JP6960932B2 - Intermediate film with improved optical properties - Google Patents

Description

[0001] This application is a partial continuation of the US patent application 14 / 563,011 currently pending on December 8, 2014, the disclosure of which is incorporated herein by reference in its entirety. Is.

[0002] The present invention relates to polymer resins, and particularly to polymer resins suitable for use in polymer interlayers such as those used in multilayer panels.

[0003] Poly (vinyl butyral) (PVB) is often used in the manufacture of polymer sheets that can be used as interlayer films in multilayer panels such as light transmissive laminates such as safety glass or polymer laminates. .. PVBs are also used in photovoltaic solar panels to enclose panels used to generate and supply electricity for commercial and residential applications.

[0004] Safety glass refers to a transparent laminate containing at least one polymer sheet or interlayer film that is generally placed between two sheets of glass. Safety glass is often used as a transparent barrier in construction and automotive applications, and one of its main functions is to absorb the energy generated from impacts or blows without penetrating the glass into an object, and the applied force is applied. Keeping the glass bonded, even if it is sufficient to break the glass. This avoids the dispersion of sharp glass shards and minimizes damage and damage to people or objects within the enclosed area. Safety glass can also provide other benefits such as reduction of ultraviolet (UV) and / or infrared (IR) radiation, which also adds color, texture, etc. to the aesthetic of window openings. The appearance can also be improved. In addition, safety glasses with the desired sound insulation properties that provide a quieter interior space are also manufactured.

[0005] Laminated safety glass is used in vehicles equipped with a head-up display (HUD) system that projects an image of the instrument group or other important information onto the position of the operator's eye level on the windshield. Has been done. Such a display allows the driver to stay focused on the approaching path while visually obtaining dashboard information. When projected onto a flat windshield with a uniform and stable thickness, the projected image reflects off the inner and outer surfaces of the glass, thus causing a double or reflective "ghost" that interferes with the difference in the position of the projected image. An image is formed.

[0006] One way to deal with these ghost images is to include a coating, such as a dielectric coating, over one of the windshield surfaces between the glass and the polymer interlayer. This coating is designed to form a third ghost image in close proximity to the primary image while significantly reducing the brightness of the secondary image so that the secondary image appears to blend into the background. There is. Unfortunately, sometimes the effectiveness of such a coating may be limited and the coating itself may interfere with the adhesion of the polymer interlayer to the glass substrate, causing optical distortion and other problems. ..

[0007] At the same time, due in part to the increased fuel efficiency demands for vehicles, the demand for multi-layer panels, which are lighter than traditional panels, is growing. Generally, multi-layer panels used in vehicles, such as their windshields, side windows, and other panels, constitute a notable portion (sometimes up to 5%) of the total weight of the vehicle. do. As a result, reducing the total weight of these panels will generally result in a reduction in vehicle weight and a concomitant increase in fuel efficiency. Most of the weight in these panels is due to the substrate (usually including glass) rather than to the intermediate layer.

[0008] Therefore, there is a need for polymer interlayers suitable for use in HUD applications that can also be used in lightweight multilayer panels. Such interlayer films must exhibit desirable optical, sound insulation, and visual properties while reducing double image separation and allowing the use of thinner substrates.

[0009] One aspect of the invention relates to a tapered interlayer containing at least one polymer layer containing a poly (vinyl acetal) resin and at least one plasticizer. The polymer layer has a refractive index of at least about 1.480 and the interlayer contains a tapered area with an overall rust angle of 0.85 mrad or less.

[0010] Another aspect of the invention relates to a multilayer panel comprising a pair of hard substrates; and an interlayer film disposed between the substrates. The interlayer film contains a tapered area with an overall wedge angle of less than 0.85 mrad, and the equivalent index of refraction of the multilayer panel is at least 0.010 higher than the respective index of refraction of the hard substrate.

[0011] Yet another aspect of the invention relates to a multilayer panel comprising a pair of hard substrates and a tapered interlayer film disposed between the substrates. The tapered interlayer contains at least one polymer resin. The index of refraction of the interlayer film is at least 5% higher than the index of refraction of each of the hard substrates.

[0012] Various aspects of the invention will be described in detail below with reference to the accompanying drawings.

[0013] FIG. 1 is a cross-sectional view of a tapered interlayer film configured according to an aspect of the present invention, labeled with various features of the tapered interlayer film for easy reference. [0014] FIG. 2 is a cross-sectional view of a tapered interlayer film having a tapered zone over the entire width of the interlayer film, the entire tapered area having a constant wedge angle and linear thickness profile. [0015] FIG. 3 shows a tapered area that covers a portion of the width of the interlayer, and a horizontal area that covers a portion of the width of the interlayer, the tapered area including a constant angle area and a variable angle area. FIG. 3 is a cross-sectional view of a tapered interlayer film having an end area of flat). [0016] FIG. 4 shows a tapered area that covers a portion of the width of the interlayer and a portion of the width of the interlayer, the tapered area including a constant angle area and two variable angle areas. FIG. 5 is a cross-sectional view of a tapered interlayer having two horizontal end areas. [0017] FIG. 5 shows a tapered area covering a portion of the width of the interlayer, and an interlayer, in which the tapered area is formed from a variable angle area having a fully curved thickness profile. FIG. 5 is a cross-sectional view of a tapered interlayer having two horizontal end areas covering a portion of its width. [0018] FIG. 6 shows a tapered interlayer having a tapered zone that spans the entire width of the interlayer, including three constant angle zones where the tapered portions are separated from each other by two variable angle zones. It is a cross-sectional view of. [0019] FIG. 7 shows a tapered area that covers a portion of the width of the interlayer and a portion of the width of the interlayer, the tapered area including three constant angle areas and four variable angle areas. It is a cross-sectional view of a tapered interlayer film having two horizontal end areas extending over. [0020] FIG. 8a is a plan view of a tapered interlayer film configured for use on the windshield of a vehicle, the thickness profile of the interlayer film being similar to the thickness profile of the interlayer film shown in FIG. .. [0021] FIG. 8b is a cross-sectional view of the interlayer film of FIG. 8a showing the thickness profile of the interlayer film. [0022] FIG. 9 is a schematic view of an apparatus used to measure the double image separation distance of a multilayer panel. [0023] FIG. 10 is an example of a projection image formed when measuring the double image separation distance of the multilayer panel using the apparatus of FIG. [0024] FIG. 11 is an example of a graph formed by analyzing the projected image shown in FIG. 10 by plotting the number of pixels as a function of intensity. [0025] FIG. 12 is a graph representation of the results of the double image separation distance analysis performed on some of the comparative samples described in Example 11 and the samples of the present invention, especially for some samples of various wedge angles. The double image separation distance is shown as a function of total thickness. [0026] FIG. 13 is a graph display of the results of the double image separation distance analysis performed on some of the comparative samples described in Example 11 and the sample of the present invention, particularly on some samples of various glass structures. The double image separation is shown as a function of the wedge angle. [0027] FIG. 14 is a graph showing the results of the double image separation distance analysis performed in Example 13, particularly showing the double image separation distances of some panels using panels with various glass thicknesses. It is shown as a function of the equivalent refractive index.

[0028] The resin composition, layer, and interlayer film according to various aspects of the present invention may contain one or more thermoplastic polymers and a refractive index (RI) adjusting agent (balancing agent). As used herein, the term "refractive index modifier" or "RI modifier" is any component that is included in a composition, layer, or interlayer film to regulate the refractive index of at least one resin or layer. Or refers to an additive. The RI modifier can increase or decrease the index of refraction of at least one of the resins or layers in the interlayer film, thereby degrading the optical properties of the interlayer film such as color spots, haze, and / or clarity. It can be improved compared to the same interlayer film formed without the use of RI modifiers.

[0029] As used herein, the terms "polymer resin composition" and "resin composition" refer to a composition containing one or more types of polymer resins. The polymer composition may optionally contain other components such as plasticizers and / or other additives. As used herein, the terms "polymer resin layer," "polymer layer," and "resin layer" refer to one or more polymer resins molded into a polymer sheet, optionally mixed with one or more plasticizers. Point to. Again, the polymer layer can contain additional additives, but these are not required. As used herein, the term "intermediate film" refers to a monolayer or multilayer polymer sheet suitable for use with at least one rigid substrate to form a multilayer panel. The terms "single sheet" interlayer film and "monolith type" interlayer film refer to an interlayer film formed from one single resin sheet, while the terms "multi-layer" and "multilayer" interlayer film refer to. Refers to an interlayer film having two or more resin sheets that are coextruded, laminated, or otherwise bonded to each other.

[0030] The resin compositions, layers, and interlayer films described herein can contain one or more thermoplastic polymers. Examples of suitable thermoplastic polymers are poly (vinyl acetal) resin, polyurethane (PU), poly (ethylene-co-vinyl) acetate (EVA), polyvinyl chloride (PVC), poly (vinyl chloride-co-methacrylate). ), Polyethylene, polyolefin, ethylene acrylate ester copolymers, poly (ethylene-co-butyl acrylate), silicone elastomers, epoxy resins, and ethylene / carboxylic acid copolymers derived from any of the polymers listed above and their ionomers. Acid copolymers and combinations thereof can be mentioned, but are not limited to these. In some embodiments, the thermoplastic polymer can be selected from the group consisting of poly (vinyl acetal) resins, polyvinyl chloride, and polyurethane, or the resin can be one or more poly (vinyl acetal) resins. Can be included. Although described herein with respect to a poly (vinyl acetal) resin, according to various aspects of the invention, one or more of the above-mentioned poly (vinyl acetal) resins described below may be used in combination with or in place of the poly (vinyl acetal) resins described below. It should be understood that polymer resins can be included.

When the resin compositions, layers, and interlayer films described herein contain a poly (vinyl acetal) resin, the poly (vinyl acetal) resin can be formed according to any suitable method. .. Poly (vinyl acetal) resins can be formed by acetalizing polyvinyl alcohol with one or more aldehydes in the presence of an acid catalyst. The resulting resins are then described, for example, in US Pat. Nos. 2,282,057 and 2,282,026, and "Vinyl Acetal Polymers", Encyclopedia of Polymer Science & Technology, 3rd Edition, vol.8, p.381-399, It can be separated, stabilized and dried according to known methods such as those described in BE Wade (2003). The resulting poly (vinyl acetal) resin is at least about 50% by weight, at least about 60% by weight, at least about 70% by weight, at least about 75% by weight as measured according to ASTM-D1396, unless otherwise indicated. It may have a total acetalization degree of at least about 80% by weight and at least about 85% by weight. The total amount of aldehyde residues in the poly (vinyl acetal) resin can be generically referred to as the acetal component, the rest of the poly (vinyl acetal) resin is the residual hydroxyl and residual acetate groups, which will be discussed in more detail below. ..

[0032] According to some embodiments, the resin composition, layer, or interlayer can contain at least one poly (vinyl acetal) resin, which is the composition, layer, or intermediate. At least about 0.5% by weight, at least about 1% by weight, at least about 2% by weight, at least about 3% by weight, at least about 5% by weight, at least about 10% by weight, at least about 10% by weight, based on the total weight of all resins in the film. It can be present in the composition, layer, or interlayer in an amount of about 15% by weight, at least about 20% by weight, at least about 30% by weight, at least about 40% by weight, or at least about 45% by weight. Overall, at least one poly (vinyl acetal) resin is at least about 10% by weight, at least about 20% by weight, at least about 30% by weight of the composition, layer, or interlayer film, based on the total weight of the total resin. , At least about 40% by weight, at least about 50% by weight, at least about 60% by weight, at least about 70% by weight, or at least about 80% by weight. In some embodiments, the amount of resin other than at least one poly (vinyl acetal) resin is about 20% by weight or less, about 15% by weight or less, about 10% by weight or less, based on the total weight of all resins. It may be about 5% by weight or less, about 2% by weight or less, or about 1% by weight or less.

[0033] In some embodiments, the resin composition, layer, or interlayer may contain at least a first poly (vinyl acetal) resin and a second poly (vinyl acetal) resin. Each of these is at least about 0.5% by weight, at least about 1% by weight, at least about 2% by weight, at least about 3% by weight, at least about 3% by weight, based on the total weight of the total resin in the composition, layer, or interlayer film. Compositions, layers, or at least about 5% by weight, at least about 10% by weight, at least about 15% by weight, at least about 20% by weight, at least about 30% by weight, at least about 40% by weight, or at least about 45% by weight. It can be present in the interlayer. Overall, the first and second poly (vinyl acetal) resins are at least about 10% by weight, at least about 20% by weight, and at least about 30% by weight of the composition, layer, or interlayer film, based on the total weight of the total resin. It can be made up of% by weight, at least about 40% by weight, at least about 50% by weight, at least about 60% by weight, at least about 70% by weight, or at least about 80% by weight. In some embodiments, the amount of resin other than the first and second poly (vinyl acetal) resins is about 20% by weight or less, about 15% by weight or less, about 10% by weight based on the total weight of all resins. Hereinafter, it may be about 5% by weight or less, about 2% by weight or less, or about 1% by weight or less.

[0034] In some embodiments, one of the first and second poly (vinyl acetal) resins is less than 12% by weight based on the total weight of the first and second poly (vinyl acetal) resins. Can be present in the composition, layer, or interlayer film. For example, the first or second poly (vinyl acetal) resin is at least about 0.5% by weight, at least about 1% by weight, at least about about, based on the total weight of the first and second poly (vinyl acetal) resins. 1.5% by weight, at least about 2% by weight, at least about 2.5% by weight, at least about 3% by weight, at least about 3.5% by weight, at least about 4% by weight, at least about 4.5% by weight, at least about about 5% by weight, at least about 5.5% by weight, at least about 6% by weight, at least about 6.5% by weight, at least about 7% by weight, and / or about 12% by weight or less, about 11.5% by weight or less, about 11% by weight or less, about 10.5% by weight or less, about 10% by weight or less, about 9.5% by weight or less, about 9% by weight or less, about 8.5% by weight or less, about 8% by weight or less, about 7. It can be present in the composition, layer, or interlayer in an amount of 5% by weight or less. In some embodiments, one of the first and second poly (vinyl acetal) resins is about 0.5 to about 12% by weight based on the total weight of the first and second poly (vinyl acetal) resins. Can be present in the composition, layer, or interlayer in an amount ranging from about 1.5 to about 11.5% by weight, about 2 to about 11% by weight, and about 2.5 to about 10% by weight. can.

[0035] The first and second poly (vinyl acetal) resins can contain residues of any suitable aldehyde, and in some embodiments at least one C _1- C ₁₀ aldehyde. , or residues of at least one _C 4 -C ₈ aldehydes can be included. Examples of suitable _C 4 -C ₈ aldehydes, n- butyraldehyde, isobutyraldehyde, 2-methyl valeraldehyde, n- hexyl aldehyde, 2-ethylhexyl aldehyde, n- octyl aldehyde, and that the combinations thereof Yes, but not limited to these. At least about 20% by weight, at least about 30% by weight, at least about 40% by weight, at least about 50% by weight, based on the total weight of the aldehyde residues of the resin, on at least one of the first and second poly (vinyl acetal) resins. %, at least about 60 wt%, or at least about 70% by weight of at least one _C 4 -C ₈ aldehydes residues can be included in, and / or from about 90 wt% or less, about 85 wt% or less, about 80 wt% or less, about 75 wt% or less, about 70 wt% or less, or about 65 weight percent of at least one _C 4 -C ₈ aldehydes, or from about 20 to about 90 wt%, from about 30 to about 80 wt%, or from about 40 to about 70 weight percent range it may be included at least one _C 4 -C ₈ aldehydes. C _{4 to} C ₈ aldehydes can be selected from the groups shown above, or they can be selected from the group consisting of n-butyraldehyde, isobutyraldehyde, 2-ethylhexyl aldehyde, and combinations thereof.

[0036] In various embodiments, the first and / or second poly (vinyl acetal) resin may be polyvinyl n-butyral (PVB) resin. In other embodiments, the first and / or second poly (vinyl acetal) resin contains predominantly n-butyraldehyde residues, eg, about 50% by weight based on the total weight of all aldehyde residues in the resin. Hereinafter, residues of aldehydes other than n-butyraldehyde of about 40% by weight or less, about 30% by weight or less, about 20% by weight or less, about 10% by weight or less, about 5% by weight or less, or about 2% by weight or less of aldehydes other than n-butyraldehyde. It may be a poly (vinyl n-butyral) resin which may be contained. When the first and / or second poly (vinyl acetal) resin is a PVB resin, the molecular weight of the resin is size-exclusion chromatography using the Low Angle Laser Light Scattering (SEC / LALLS) method of Cottons and Ouano. At least about 50,000 daltons, at least about 70,000 daltons, at least about 100,000 daltons, and / or about 600,000 daltons or less, about 550,000 daltons or less, about 500,000 daltons or less, about It may be 450,000 daltons or less, or 425,000 daltons or less. As used herein, the term "molecular weight" refers to weight average molecular weight (M _w ). The molecular weight of the first and / or second poly (vinyl acetal) resin is about 50,000 to about 600,000 daltons, about 70,000 to about 450,000 daltons, or about 100,000 to about 425,000. It may be in the Dalton range.

[0037] Although generally described herein with respect to first and second poly (vinyl acetal) resins, in some embodiments an equivalent single poly (vinyl acetal) resin containing first and second acetal groups. It should be understood that similar results can be obtained by substituting the first and second poly (vinyl acetal) resins. As used herein, the term "poly (vinyl acetal) resin composition" may refer to individual poly (vinyl acetal) resins present in a blend of resins, or a single poly (vinyl acetal) resin. It may refer to the acetal group present above. In various embodiments, the weight ratio of the amount of the first poly (vinyl acetal) resin component to the second poly (vinyl acetal) resin component in the layer, interlayer, or blend is about 0.5:99. .5-about 99.5: 0.5, about 1:99-99: 1, about 10:90-about 90:10, about 25:75-about 75:25, or about 40:60-about 60: It may be in the range of 40.

[0038] In some embodiments, the at least one resin composition, layer, or interlayer film comprises at least a first poly (vinyl acetal) resin component and a second poly (vinyl acetal) resin component. Can be done. In some embodiments, the first and second resin components may contain first and second poly (vinyl acetal) resins, which may be physically mixed to form a resin blend. It can be mixed with one or more plasticizers or other additives to give a blended polymer layer or interlayer film. In other embodiments, the first and second poly (vinyl acetal) resin components can be present as first and second acetal moieties in a single poly (vinyl acetal) resin, respectively. Similar to resin blends, this single "composite" poly (vinyl acetal) resin can optionally be blended with a plasticizer for use in polymer layers and interlayer films.

[0039] In some embodiments, when the resin component contains a poly (vinyl acetal) resin, the first and second poly (vinyl acetal) resins are such that one of the first and second resins is the first. Dispersed in the other of the first and second resins to form one domain of the first and second poly (vinyl acetal) resins in the other of the first and second poly (vinyl acetal) resins. Can be blended as it can be. The blended resin can be used as a single layer interlayer, or it can be combined with one or more adjacent layers to form a multilayer interlayer. In another embodiment, the first and second poly (vinyl acetal) resins are present in adjacent layers of the multilayer interlayer, and one of the plurality of layers of the interlayer is the first poly (vinyl acetal). It may contain a resin so that the other layer of the interlayer contains a second poly (vinyl acetal) resin. Further, an additional layer may be present adjacent to at least one of the plurality of layers.

[0040] The resin composition, layer, and interlayer film according to the various aspects of the present invention may further contain at least one type of plasticizer. Depending on the particular composition of one or more resins in the composition, layer, or interlayer film, the plasticizer is at least about 5 phr, at least about 10 phr, at least about 15 phr, at least about 15 phr, per 100 parts of resin. About 20 phr, at least about 25 phr, at least about 30 phr, at least about 35 phr, at least about 40 phr, at least about 45 phr, at least about 50 phr, at least about 55 phr, at least about 60 phr, and / or about 120 phr or less, about 110 phr or less, about 105 phr or less, About 100 phr or less, about 95 phr or less, about 90 phr or less, about 85 phr or less, about 75 phr or less, about 70 phr or less, about 65 phr or less, about 60 phr or less, about 55 phr or less, about 50 phr or less, about 45 phr or less, or about 40 phr or less, or It can be present in an amount in the range of about 5 to about 120 phr, about 10 to about 110 phr, about 20 to about 90 phr, or about 25 to about 75 phr. Specific embodiments will be discussed in detail below.

[0041] As used herein, the term "parts per 100 parts of resin" or "phr" refers to the amount of plasticizer present relative to 100 parts of resin on a weight basis. For example, when 30 g of the plasticizer is added to 100 g of the resin, the plasticizer is present in an amount of 30 phr. When the resin composition, layer, or interlayer film contains two or more kinds of resins, the weight of the plasticizer is compared with the total amount of all existing resins to determine the portion per 100 parts of the resin. Further, where the plasticizer content of the layer or interlayer is given herein, it is given with respect to the amount of plasticizer in the mixture or melt used to make the layer or interlayer. There is.

[0042] Examples of suitable plasticizers include triethylene glycol di (2-ethylhexanoate) (3GEH), triethylene glycol di (2-ethylbutyrate), triethylene glycol diheptanoate, tetraethylene. Glycoldiheptanoate, tetraethylene glycol di (2-ethylhexanoate) (4-GEH), dihexyl adipate, dioctyl adipate, hexylcyclohexyl adipate, diisononyl adipate, heptylnonyl adipate, di (butoxyethyl) adipate, and bis Examples include, but are not limited to, (2- (2-butoxyethoxy) ethyl) adipate, dibutyl sebacate, dioctyl sebacate, and mixtures thereof. The plasticizer can be selected from the group consisting of triethylene glycol di (2-ethylhexanoate) and tetraethylene glycol di (2-ethylhexanoate), or the plasticizer is triethylene glycol di (2-ethylhexanoate). Ethylhexanoate) may be included.

[0043] According to some embodiments, the compositions, layers, and interlayer films described herein may have different compositions of the first and second poly (vinyl acetal) resins. For example, in some embodiments, the first poly (vinyl acetal) resin is at least about 2% by weight and at least about 3% by weight of the residual hydroxyl and / or residual acetate content of the second poly (vinyl acetal) resin. %, At least about 4% by weight, at least about 5% by weight, at least about 6% by weight, or at least about 8% by weight, which may have a high or low residual hydroxyl content and / or a residual acetate content. As used herein, the terms "residual hydroxyl content" and "residual acetate content" refer to the amount of hydroxyl and acetate groups remaining on the resin after the treatment is complete, respectively. For example, polyvinyl n-butyral can be produced by hydrolyzing polyvinyl acetate to polyvinyl alcohol and then acetalizing polyvinyl alcohol with n-butyraldehyde to form polyvinyl n-butyral. In the process of hydrolyzing polyvinyl acetate, not all acetate groups are converted to hydroxyl groups, but residual acetate groups remain on the resin. Similarly, in the process of acetalizing polyvinyl alcohol, not all hydroxyl groups are converted to acetal groups, and similarly, residual hydroxyl groups remain on the resin. As a result, most poly (vinyl acetal) resins contain both a residual hydroxyl group (as a vinyl hydroxyl group) and a residual acetate group (as a vinyl acetate group) as part of the polymer chain. The residual hydroxyl content and residual acetate content are expressed in weight% based on the weight of the polymer resin and are measured according to ASTM-D1396 unless otherwise indicated.

Also, the difference between the residual hydroxyl content of the first and second poly (vinyl acetal) resins is at least about 2% by weight, at least about 5% by weight, at least about 10% by weight, and at least about 12% by weight. , At least about 15% by weight, at least about 20% by weight, or at least about 30% by weight. As used herein, the terms "... weight% different" or "difference is at least ... weight%" are two given weights calculated by subtracting one number from the other. Refers to the difference between%. For example, a poly (vinyl acetal) resin having a residual hydroxyl content of 12% by weight has a residual hydroxyl content 2% by weight lower than a poly (vinyl acetal) resin having a residual hydroxyl content of 14% by weight (14% by weight-). 12% by weight = 2% by weight). The term "difference" as used herein can refer to a value that is higher or lower than other values.

At least one of the first and second poly (vinyl acetal) resins is at least about 14% by weight, at least about 14.5% by weight, at least about 15% by weight, at least about 15.5% by weight, at least about about. 16% by weight, at least about 16.5% by weight, at least about 17% by weight, at least about 17.5% by weight, at least about 18% by weight, at least about 18.5% by weight, at least about 19% by weight, at least about 19. 5% by weight and / or about 45% by weight or less, about 40% by weight or less, about 35% by weight or less, about 33% by weight or less, about 30% by weight or less, about 27% by weight or less, about 25% by weight or less, about 22% by weight or less, about 21.5% by weight or less, about 21% by weight or less, about 20.5% by weight or less, or about 20% by weight or less, or about 14 to about 45% by weight, about 16 to about 30% by weight. , May have a residual hydroxyl content in the range of about 18 to about 25% by weight, about 18.5 to about 20% by weight, or about 19.5 to about 21% by weight.

[0046] Other poly (vinyl acetal) resins are at least about 8% by weight, at least about 9% by weight, at least about 10% by weight, at least 11% by weight, and / or about 16% by weight or less, about 15% by weight or less. , About 14.5% by weight or less, about 13% by weight or less, about 11.5% by weight or less, about 11% by weight or less, about 10.5% by weight or less, about 10% by weight or less, about 9.5% by weight or less Or may have a residual hydroxyl content in the range of about 9% by weight or less, or about 8 to about 16% by weight, about 9 to about 15% by weight, or about 9.5 to about 14.5% by weight. The difference between the residual hydroxyl contents of the first and second poly (vinyl acetal) resins can be selected to be at least about 2% by weight as described above. Also, one or more other poly (vinyl acetal) resins can be present in the resin composition, layer, or interlayer film, which may have residual hydroxyls within the range given above. Further, the residual hydroxyl content of one or more other poly (vinyl acetal) resins may be the same as or different from the residual hydroxyl content of the first and / or second poly (vinyl acetal) resins.

[0047] In some embodiments, at least one of the first and second poly (vinyl acetal) resins may have a residual acetate content different from the other. For example, in some embodiments, the difference between the residual acetate content of the first and second poly (vinyl acetal) resins is at least about 2% by weight, at least about 3% by weight, at least about 4% by weight, at least about about. It may be 5% by weight, at least about 8% by weight, and at least about 10% by weight. One of the poly (vinyl acetal) resins has a residual acetate content of about 4% by weight or less, about 3% by weight or less, about 2% by weight or less, or about 1% by weight or less as measured as described above. You may be. In some embodiments, at least one of the first and second poly (vinyl acetal) resins is at least about 5% by weight, at least about 8% by weight, at least about 10% by weight, at least about 12% by weight, at least about about. It may have a residual acetate content of 14% by weight, at least about 16% by weight, at least about 18% by weight, at least about 20% by weight, or at least about 30% by weight. The difference in residual acetate content between the first and second poly (vinyl acetal) resins may be within the range given above, or the difference may be less than about 3% by weight, about 2% by weight or less, about 1 It may be less than or equal to% by weight, or less than or equal to about 0.5% by weight. The additional poly (vinyl acetal) resin present in the resin composition or interlayer film has a residual acetate content that is the same as or different from the residual acetate content of the first and / or second poly (vinyl acetal) resin. You can.

[0048] In some embodiments, the difference between the residual hydroxyl content of the first and second poly (vinyl acetal) resins is less than about 2% by weight, less than about 1% by weight, about 0.5% by weight. The difference in residual acetate content between the first and second poly (vinyl acetal) resins may be at least about 3% by weight, at least about 5% by weight, at least about 8% by weight, and at least about 15% by weight. %, At least about 20% by weight, or at least about 30% by weight. In other embodiments, the difference in residual acetate content between the first and second poly (vinyl acetal) resins is less than about 3% by weight, about 2% by weight or less, about 1% by weight or less, or about 0.5% by weight. The difference in residual hydroxyl content between the first and second poly (vinyl acetal) resins may be at least about 2% by weight, at least about 5% by weight, at least about 10% by weight, and at least about 12% by weight. , At least about 15% by weight, at least about 20% by weight, or at least about 30% by weight.

[0049] In various embodiments, the difference in residual hydroxyl and / or residual acetate content of the first and second poly (vinyl acetal) resins is strength, resistance to the final composition, layer, or interlayer film. It can be selected to control or provide some performance characteristics such as impact resistance, penetration resistance, workability, or sound insulation performance. For example, a poly (vinyl acetal) resin having a higher residual hydroxyl content, typically greater than about 16% by weight, can promote high impact resistance, penetration resistance, and strength to the resin composition or layer, while Resins with lower hydroxyl content, typically having a residual hydroxyl content of less than 16% by weight, can improve the sound insulation performance of interlayer films or blends.

[0050] Poly (vinyl acetal) resins having a higher or lower residual hydroxyl content and / or residual acetate content will also eventually have different amounts of plasticizer when mixed with at least one plasticizer. Can be included. As a result, layers or domains formed from first and second poly (vinyl acetal) resins with different compositions can also have different properties in a single polymer layer or interlayer film. Although not bound by theory, it is estimated that the compatibility of a given plasticizer with a poly (vinyl acetal) resin may be determined, at least in part, by the composition of the polymer, and in particular its residual hydroxyl content. Will be done. In general, poly (vinyl acetal) resins with higher residual hydroxyl content tend to show lower compatibility (or volume) to a given plasticizer than similar resins with lower residual hydroxyl content. be. As a result, poly (vinyl acetal) resins with higher residual hydroxyl content tend to be less plasticized and exhibit higher flexibility than similar resins with lower residual hydroxyl content. Conversely, poly (vinyl acetal) resins with lower residual hydroxyl content may tend to introduce higher amounts of plasticizer when plasticized with a given plasticizer. A softer polymer layer may be provided that exhibits a lower glass transition temperature than a polymer layer containing a similar resin with a higher residual hydroxyl content. Depending on the particular resin and plasticizer, these trends can be reversed.

[0051] When two poly (vinyl acetal) resins with different levels of residual hydroxyl content are blended with the plasticizer, the plasticizer is partitioned between the polymer layers or domains to form a layer with a lower residual hydroxyl content or. More plasticizer can be present in the domain and less plasticizer can be present in the layer or domain with the higher residual hydroxyl content. Eventually, an equilibrium state is achieved between the two resins. The correlation between the residual hydroxyl content of the poly (vinyl acetal) resin and the plasticizer compatibility / volume can facilitate the addition of an appropriate amount of plasticizer to the polymeric resin. This correlation also facilitates stable maintenance of the difference in plasticizer content between the two or more resins when the plasticizer is transferred between the resins in other forms.

[0052] In some embodiments, the polymer layer or interlayer has at least a first polymer layer containing a first poly (vinyl acetal) resin and a first plasticizer, and a second poly (vinyl). A second polymer layer adjacent to the first polymer layer can be included, which comprises an acetal) resin and a second plasticizer. The first plasticizer and the second plasticizer may be the same type of plasticizer, or the first plasticizer and the second plasticizer may be different. In some embodiments, at least one of the first and second plasticizers may be a blend of two or more plasticizers, which may be the same or different from one or more other plasticizers. Difference in plasticizer content between polymer layers when one of the first and second poly (vinyl acetal) resins has a residual hydroxyl content that is at least 2% by weight or lower than the residual hydroxyl content of the other. May be at least about 2 phr, at least about 5 phr, at least about 8 phr, at least about 10 phr, at least about 12 phr, or at least about 15 phr. In most embodiments, the polymer layer containing the resin with the lower hydroxyl content may have a higher plasticizer content. In order to control or maintain the other properties of the polymer layer or interlayer film, the difference in plasticizer content between the first and second polymer layers is about 40 phr or less, about 30 phr or less, about 25 phr or less, about 20 phr. It may be less than or equal to, or about 17 phr or less. In other embodiments, the difference in plasticizer content between the first and second polymer layers may be at least about 40 phr, at least about 50 phr, at least about 60 phr, or at least about 70 phr.

As a result, in some embodiments where the first and second poly (vinyl acetal) resins are present in adjacent layers of the multilayer interlayer, the first and second polymer layers have different glass transitions. It may indicate the temperature. Similarly, when the first and second poly (vinyl acetal) resins are present in the blend, one domain of the first and second poly (vinyl acetal) resins is the first and second poly. It may show a glass transition temperature different from that of the other (vinyl acetal) resin. The glass transition temperature or T _g is a temperature indicating the transition of the polymer from the glass state to the rubber state. The glass transition temperatures of the resins and layers described herein were determined by dynamic mechanical thermal analysis (DMTA). DMTA is a sample storage (elastic) coefficient (G') (Pascal), loss (viscosity) coefficient (G ") (Pascal), and tan δ (G" / G'), given frequency and temperature sweep. Measured as a function of temperature in velocity. Next, the glass transition temperature is determined by the position of the tan δ peak on the temperature scale. The glass transition temperature given here was determined at a temperature sweep rate of 3 ° C./min under the shear mode at a frequency of 1 Hz.

[0054] The difference in glass transition temperature between the various regions of the first polymer layer and the second polymer layer, or the blended resin or polymer layer, is at least about 3 ° C, at least about 5 ° C, at least about 8. ° C., at least about 10 ° C., at least about 12 ° C., at least about 15 ° C., at least about 18 ° C., at least about 20 ° C., at least about 22 ° C., or at least about 25 ° C. One of the first and second polymer layers is at least about 26 ° C, at least about 28 ° C, at least about 30 ° C, at least about 33 ° C, at least about 35 ° C, and / or about 70 ° C or less, about 65 ° C or less, It may have a glass transition temperature in the range of about 60 ° C. or lower, about 55 ° C. or lower, about 50 ° C. or lower, or about 26 to about 70 ° C., about 30 to about 60 ° C., and about 35 to about 50 ° C. The other of the first and second poly (vinyl acetal) resins is 25 ° C or lower, about 20 ° C or lower, about 15 ° C or lower, about 10 ° C or lower, about 5 ° C or lower, about 0 ° C or lower, about -5 ° C or lower. Or may have a glass transition temperature of about −10 ° C. or lower.

[0055] When blending the first and second poly (vinyl acetal) resins with each other so that the domains of one resin are dispersed in the other, the domains of the first and second resins. There can also be such a difference in plasticizer content and / or glass transition temperature between the two. For example, in some embodiments, the polymer layer or interlayer has various domains with higher or lower plasticizer content and / or higher or lower glass transition temperatures, as described above. Domains can be included. In some embodiments, at least a portion of the polymer layer or interlayer is at least about 26 ° C., at least about 28 ° C., at least about 30 ° C., at least about 33 ° C., at least about 35 ° C., and / or about 70 ° C. or less. Has a glass transition temperature in the range of about 65 ° C. or lower, about 60 ° C. or lower, about 55 ° C. or lower, about 50 ° C. or lower, or about 26 to about 70 ° C., about 28 to about 60 ° C., about 35 to about 50 ° C. And / or at least part of the polymer layer or interlayer film is 25 ° C or lower, about 20 ° C or less, about 15 ° C or less, about 10 ° C or less, about 5 ° C or less, about 0 ° C or less, about − It may have a glass transition temperature of 5 ° C. or lower, or −10 ° C. or lower.

[0056] One or more resin blends, layers, and interlayer films described herein can be impregnated with various other additives to impart specific properties or characteristics to the interlayer film. Such additives include dyes, pigments, stabilizers such as UV stabilizers, antioxidants, antiblocking agents, flame retardants, IR absorbers or blocking agents such as indium tin oxide, antimonth tin oxide, lanthanum hexaborate (s). LaB ₆ ), and cesium tungsten oxide, processing aids, flow-improving additives, lubricants, impact resistance improvers, nucleating agents, heat stabilizers, UV absorbers, dispersants, surfactants, chelating agents, cups Rings, adhesives, primers, strengthening additives, and fillers can be mentioned, but are not limited to these.

[0057] Further, various adhesion control agents (ACAs) can be used in the interlayer film of the present invention to control the adhesiveness of the sheet to glass. In various embodiments, the amount of ACA present in the resin composition, layer, or interlayer is at least about 0.003 phr, at least about 0.01 phr, at least about 0.025 phr, and / or about 0.15 phr or less. , About 0.10 phr or less, or about 0.04 phr or less, or about 0.003 to about 0.15 phr, about 0.01 to about 0.10 phr, or about 0.025 to about 0.04 phr. good. Suitable ACA are disclosed in sodium acetate, potassium acetate, magnesium bis (2-ethylbutyrate), magnesium bis (2-ethylhexanoate), and combinations thereof, as well as in US Pat. No. 5,728,472. ACA can be mentioned, but is not limited to these.

[0058] Resins with different compositions and thermoplastic polymer layers with different properties also tend to exhibit different indices of refraction, which can reduce the optical quality of the resulting layer or blend. Although not bound by theory, such differences in index of refraction can cause light passing through different polymer layers or domains to refract in different directions, which can cause fogging in the final product. it is conceivable that. Sometimes the absolute value of the difference between the index of refraction of the first poly (vinyl acetal) resin or layer and the index of refraction of the second poly (vinyl acetal) resin or layer is at a wavelength of 589 nm and 25 according to ASTM-D542. It may exceed 0.010 as measured at ° C. As a result, these compositions, layers, or interlayers can have cloudiness greater than 5% and / or color spot values greater than 3.

[0059] However, in various aspects of the present invention, in addition to the composition, layer, and interlayer film containing the poly (vinyl acetal) resin, at least in order to adjust the refractive index of the composition, layer, or interlayer film. One type of refractive index (RI) modifier can be included. In some embodiments, the composition, layer, or interlayer film contains at least a first poly (vinyl acetal) resin and a second poly (vinyl acetal) resin, together with at least one RI modifier. Can be included. In other embodiments, the composition, layer, or interlayer film can contain a single poly (vinyl acetal) resin with at least one RI regulator. As discussed above, the RI modifier increases or decreases the index of refraction of at least one resin or layer, thereby giving the optical properties of the interlayer film the same interlayer film formed without the RI modifier. It may be any suitable agent present in the resin or resin blend, layer, or interlayer film, or a portion thereof, which can be improved as compared to. In some embodiments, the resin blend, layer, or interlayer may have a cloudiness of at least 5% when formed in the absence of an RI modifier.

[0060] The RI modifier may be in any suitable form and can be physically blended with one or more resins, or chemically bound or reacted with at least one resin to make an RI modifier. The agent can be introduced into the polymer chain. Examples of RI modifiers include, but are limited to, liquid RI additives, solid RI additives, and residues of at least one aldehyde present in one or more of poly (vinyl acetal) resins. Not done. Here, various aspects of RI modifiers and resin compositions, layers, and interlayers containing them will be discussed in detail below.

[0061] The RI modifier can be present in the resin, polymer layer, or interlayer film in an amount sufficient to alter the refractive index of the poly (vinyl acetal) resin, polymer layer, or interlayer film. The RI modifier also changes the index of refraction of at least one of the two poly (vinyl acetal) resins, thereby minimizing the difference between the indices of the two poly (vinyl acetal) polymer layers having different indices. It can also be present in the composition, layer, or interlayer in sufficient quantity. The RI modifier can also minimize the difference between the refractive index of one or more poly (vinyl acetal) resins and one or more plasticizers in the resin composition, layer, or interlayer film. In some embodiments, the RI modifier sets the absolute value of the difference between the refractive index of the first poly (vinyl acetal) polymer layer and the refractive index of the second poly (vinyl acetal) polymer layer to 0. To reduce to 010 or less, about 0.009 or less, about 0.008 or less, about 0.007 or less, about 0.006 or less, about 0.005 or less, about 0.004 or less, or about 0.003 or less It can be present in sufficient quantity. When the multilayer interlayer contains two or more polymer layers, the RI modifier can be present in one or both layers, and in some embodiments, one or more other in one layer. It can be present in a larger amount than in the layer of.

[0062] In some embodiments, the RI modifier comprises one or more residues of an aldehyde having a refractive index of at least 1.421 as measured by ASTM-D542 at a wavelength of 589 nm and a temperature of 25 ° C. You can stay. This RI-adjusted aldehyde (also referred to herein as "high refractive index aldehyde" or "high RI aldehyde") is at least about 1.425, at least about 1.450, at least about 1.475, at least about 1.500. , At least about 1.510, or at least about 1.515, and / or about 1.675 or less, about 1.650 or less, or about 1.625 or less, or about 1.425 to about 1.675, about 1. It may have a refractive index in the range of 475 to about 1.650, or about 1.515 to about 1.625. The high RI aldehyde may be an aromatic aldehyde containing at least one aromatic ring or group. Examples of aromatic aldehydes include, but are not limited to _{, C 7 to} C ₃₀ aromatic aldehydes, C _{8 to} C ₂₅ aromatic aldehydes, or C _{9 to} C _{20 aromatic aldehydes.} Specific examples of high RI aldehydes that can be used as RI modifiers in various aspects of the present invention are shown in Table 1 below.

[0063] If the RI modifier contains a residue of at least one high RI aldehyde, then at least one of the first and second poly (vinyl acetal) resins will have a first or second poly (vinyl acetal) resin. ) At least about 0.5%, at least about 1%, at least about 5%, at least about 10%, at least about 15%, at least about 20%, at least about 25%, at least based on the total weight of the aldehyde residues in the resin. About 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, at least about 75%, at least About 80%, at least about 85%, at least about 90%, at least about 95%, and / or about 99.5% by weight or less, about 99% by weight or less, about 97% by weight or less, about 95% by weight or less, about 90 At least one type of high RI aldehyde in an amount of less than or equal to, about 85% by weight, about 80% by weight or less, about 75% by weight or less, about 70% by weight or less, about 65% by weight or less, or about 60% by weight or less. Residues can be included. About 0.5 to about 99.5% by weight based on the total weight of aldehyde residues of the first or second poly (vinyl acetal) resin in at least one of the first and second poly (vinyl acetal) resins. , About 10 to about 90% by weight, about 25 to about 75% by weight, or about 40 to about 60% by weight of at least one high RI aldehyde residue can be included.

[0064] The amount of high RI aldehyde residues can be determined using a combination of Fourier Transform Infrared Spectroscopy (FT-IR) and Size Exclusion Chromatography (SEC) with UV detection. In particular, FT-IR is used to measure the residual hydroxyl content of the resin, SEC is used to determine the amount of high RI aldehyde residues, and the amount of any other aldehyde residue is determined by the difference. FT-IR analysis is performed using a Perkin Elmer Spectrum 100 FT-IR spectrometer equipped with an ATR sampling attachment (commercially available from Perkin Elmer, Waltham, Massachusetts). The analysis is performed using 8 scans with a resolution of ^{4 cm -1.} Prior to the test, calibration data are obtained from several poly (vinyl n-butyral) samples with various residual hydroxyl contents that have been dried overnight at room temperature in a silica-based desiccator to remove excess moisture. The peak maximum wavenumber of the hydroxyl expansion band correlates with the vinyl alcohol molar content of each sample previously determined by ASTM-D1396, and the residual hydroxyl molar content of the sample to be analyzed using the resulting linear curve fitting. Predict. These values can be converted to% by weight by calculation after completing the determination of the composition of the poly (vinyl acetal) resin using SEC analysis, as described below.

[0065] SEC analysis is a Waters 410 in-line differential refractometer and Waters 2998PDA with Dionex Chromeleon v.6.8 data acquisition software (commercially available from Thermo Fischer Scientific, Sunnyvale, CA) with an expansion pack. This is done using a Waters 2695 Alliance pump equipped with an in-line UV detector and an automatic sampler (commercially available from Waters Corporation, Milford, Massachusetts). Analysis is performed using a PL Gel Mixed C (5 micron) column and a Mixed E (3 micron) column with an injection volume of 50 microliters at a flow rate of 1.0 mL / min. Samples are prepared by dissolving between 0.03 and 0.09 grams of resin in 10 to 15 mL of stabilized tetrahydrofuran and then filtering each through a 0.22 micron PTFE filter. Initial calibration of the chromatograph was performed using a narrow molecular weight polystyrene standard sample and a poly (vinyl acetal) resin containing only high RI aldehyde residues, and a wide molecular weight polystyrene (American Polymer Standard Corporation, Mentor, Ohio) as PSBR250K. Calibrate subsequent samples with (commercially available).

[0066] In some embodiments, only one of the first and second poly (vinyl acetal) resins contains residues of high RI aldehydes, while in other embodiments, residues across both resins. Can be included. The index of refraction of a resin containing a residue of high RI aldehyde is at least about 1.492, at least about 1.495, at least about 1.500, at least about 1.505, at least about 1.510, or at least about 1.515. May be.

[0067] In various embodiments, at least one of the first and second poly (vinyl acetal) resins may contain a residue of at least one aldehyde having a refractive index of less than 1.421. Examples of these aldehydes may for example include aliphatic aldehydes such as C ₄ -C ₈ aldehydes discussed above. Aldehydes having a refractive index of less than 1.421 can be selected from the group consisting of n-butyraldehyde, isobutyraldehyde, and 2-ethylhexylaldehyde.

[0068] When these residues are present, the total weight of the aldehyde residues of the first or second poly (vinyl acetal) resin is added to the first and / or second poly (vinyl acetal) resin. As a reference, at least about 10%, at least about 15%, at least about 20%, at least about 25%, at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55 %, At least about 60%, at least about 65%, at least about 70%, at least about 75%, at least about 80%, at least about 85%, at least about 90%, at least about 95%, and / or about 99% by weight or less , About 97% by weight or less, about 95% by weight or less, about 90% by weight or less, about 85% by weight or less, about 80% by weight or less, about 75% by weight or less, about 70% by weight or less, about 65% by weight or less, or About 60% by weight or less of these aldehydes can be included.

[0069] The amount of aldehyde residue having a refractive index of less than 1.421 was determined using the FT-IR / SEC method described above, and then the following formula: [100% by weight-weight of residual hydroxyl] % (From FT-IR) -Weight% of high RI aldehyde residues (from SEC) -Weight% of residual acetate (from FT-IR) = Weight% of aldehyde residues with a refractive index of less than 1.421] It is obtained by calculating according to. The first and / or second poly (vinyl acetal) resin contains aldehyde residues having a refractive index of less than 1.421, and the first or second poly (vinyl acetal) resin contains all the aldehyde residues. It can be included in an amount in the range of about 10 to about 99% by weight, about 25 to about 75% by weight, or about 40 to about 60% by weight based on the weight. The refractive index of one of these resins may be less than about 1.492, less than about 1.491, or less than about 1.490 as measured as described above.

[0070] According to some embodiments, one of the first and second poly (vinyl acetal) resins contains predominantly high RI aldehyde residues, while the first and second poly (vinyl acetal) resins. The other of the above contains residues of at least one aldehyde having a refractive index of less than 1.421. The term "mainly" as used herein means at least 75% by weight, and therefore a poly (vinyl acetal) resin containing primarily defined aldehyde residues shall be at least relative to the total weight of the aldehyde residues in the resin. Contains 75% by weight of defined aldehyde residues. For poly (vinyl acetal) resins containing mainly high RI aldehyde residues, about 25% by weight or less, about 20% by weight or less, about 15% by weight or less, and about 10% by weight based on the total weight of the aldehyde residues of the resin. Residues of other aldehydes having a refractive index of less than 1.421, such as% or less, about 5% by weight or less, about 2% by weight or less, or about 1% by weight or less, can be included.

Similarly, other poly (vinyl acetal) resins, which may contain aldehyde residues primarily having a refractive index of less than 1.421, are about 25 weights relative to the total weight of the aldehyde residues in the resin. % Or less, about 20% by weight or less, about 15% by weight or less, about 10% by weight or less, about 5% by weight or less, about 2% by weight or less, or about 1% by weight or less of high RI aldehyde residues. Has a refractive index of less than 1.421, at least about 75%, at least about 80%, at least about 85%, at least about 90%, at least about 95%, at least about 97%, or at least about 99% 1 It can contain more than one type of aldehyde residue. In some embodiments, the ratio of the resin containing predominantly high RI aldehyde residues in the composition to one or more other resins is at least about 1:99, at least about 5:95, and at least about 10. : 90, at least about 20:80, at least about 25:75, at least about 30:70, at least about 40:60, and / or about 99: 1 or less, about 95: 5 or less, about 90:10 or less, about 85 : 15 or less, about 75:25 or less, about 70:30 or less, or about 60:40 or less, or about 1:99 to 99: 1, about 10:90 to about 90:10, about 25:75 to 75: It may be in the range of 25, or about 40:60 to 60:40.

[0072] In other embodiments, at least one of the first and second poly (vinyl acetal) resins comprises a residue of a high RI aldehyde and at least one aldehyde having a refractive index of less than 1.421. It forms a "composite" resin containing both high and low RI aldehyde residues. According to these embodiments, the amount of high RI aldehyde residues and aldehyde residues having a refractive index of less than 1.421 in the composite resin, as well as the weight ratio of one to the other, are given above for the resin blend. It may be within the same range as. If the first or second poly (vinyl acetal) resin contains residues of both high RI and lower RI aldehydes, the other of the two poly (vinyl acetal) resins will also contain at least one of the following. It can also contain residues of high RI aldehydes. Alternatively, the other of the two resins contains little or no high RI aldehyde residue, which is less than about 10% by weight, less than about 5% by weight, less than about 2% by weight, or about. Contains less than 1% by weight of high RI aldehyde residues, the rest less than 1.421, such as n-butyraldehyde, isobutyraldehyde, 2-ethylhexyl aldehyde, and aldehydes selected from the group consisting of combinations thereof. It can be a residue of an aldehyde having a refractive index of.

[0073] If the interlayer is a multilayer interlayer, it comprises at least one polymer layer having at least a first poly (vinyl acetal) resin, and at least a second poly (vinyl acetal) resin. Other polymer layers can be included, where the difference between the residual hydroxyl content of the first poly (vinyl acetal) resin and the second poly (vinyl acetal) resin is at least 2% by weight. One or both of the poly (vinyl acetal) resins can contain residues of high RI aldehydes, one of the polymer layers being at least about 0.002, at least about 0.003, at least about 0.004, and. / Or about 0.010 or less, about 0.009 or less, about 0.008 or less, or only about 0.007 or less, or about 0.002 to about 0.010, about 0.003 to about 0.009, or It may have higher or lower refractive index by an amount in the range of about 0.004 to about 0.007. In some embodiments, the innermost polymer layer may have a higher index of refraction if the interlayer film comprises at least three polymer layers, while in other embodiments, the outer polymer layer. The refractive index of one or both of the above can be made higher. In some embodiments, only one of the first and second poly (vinyl acetal) resins can contain a residue of high RI aldehyde. In other embodiments, both poly (vinyl acetal) resins can contain residues of at least one high RI aldehyde, but the resin still exhibits a difference in index of refraction within the range given above. Can be done.

[0074] One or both of the poly (vinyl acetal) resins can contain residues of at least one high RI aldehyde. In some embodiments, where the poly (vinyl acetal) resin containing such residues has a residual hydroxyl content of, for example, 15% by weight or less, the polymer layers containing such resins are each measured as described above. Less than 20 ° C, about 15 ° C or less, about 10 ° C or less, about 5 ° C or less, about 0 ° C or less, about -5 ° C or less, or about -10 ° C or less glass transition temperature, and at least about 1.465, at least About 1.470, at least about 1.475, at least about 1.480, at least about 1.485, at least about 1.490, at least about 1.495, at least about 1.500, at least about 1.510, at least about 1 .520, at least about 1.525, at least about 1.540, at least about 1.550, at least about 1.575, at least about 1.590, at least about 1.600, at least about 1.615, at least about 1.625 , Or can have a refractive index of at least about 1.650. The plasticizer content of the layer is at least about 50 phr, at least about 55 phr, at least about 60 phr, at least about 65 phr, and / or about 120 phr or less, about 110 phr or less, about 90 phr or less, about 85 phr or less, about, according to various embodiments. It may be in the range of 80 phr or less, or about 75 phr or less, or about 50 to about 120 phr, about 55 to about 110 phr, about 60 to about 90 phr, or about 65 to about 75 phr.

[0075] If the resin having a high RI aldehyde residue in the multilayer interlayer film discussed above has a residual hydroxyl content higher than, for example, 16% by weight, the polymer layers containing this resin are described above, respectively. As measured, the glass transition temperature is at least about 26 ° C., at least about 30 ° C., at least about 33 ° C., or at least about 35 ° C., and at least about 1.470, at least about 1.475, at least about 1.480, at least. About 1.485, at least about 1.490, at least about 1.495, at least about 1.500, at least about 1.510, at least about 1.520, at least about 1.525, at least about 1.540, at least about 1 It can have a refractive index of .550, at least about 1.575, at least about 1.590, at least about 1.600, at least about 1.615, at least about 1.625, or at least about 1.650. The plasticizer content of the layer may be less than 50 phr, less than about 45 phr, less than about 40 phr, less than about 30 phr, less than about 20 phr, according to some embodiments.

The index of refraction of the entire interlayer film is at least about 1.477, at least about 1.478, at least about 1.480, at least about 1.485, at least about 1.490, as measured as described above. At least about 1.495, at least about 1.500, at least about 1.505, at least about 1.510, at least about 1.515, at least about 1.520, at least about 1.540, at least about 1.550, at least about 1.575, at least about 1.580, at least about 1.590, at least about 1.600, at least about 1.610, at least about 1.620, at least about 1.630, at least about 1.640, or at least about 1. It can be .650.

[0077] According to various aspects of the present invention, the RI modifier can include a liquid RI modifier. The term "liquid RI regulator" as used herein refers to a liquid RI regulator under standard conditions of 25 ° C. and 1 atm. In some embodiments, the liquid RI modifier may be, for example, a high RI plasticizer. The term "high RI plasticizer" as used herein refers to a plasticizer having a refractive index of at least 1.460 as measured above. High RI plasticizers suitable for use as RI modifiers are at least about 1.470, at least about 1.480, at least about 1.490, at least about 1.500, at least about about 1.470 as measured above. It may have a refractive index of 1.510, at least about 1.520, and / or about 1.600 or less, about 1.575 or less, or about 1.550 or less. The refractive index of high RI plasticizers ranges from about 1.460 to about 1.600, about 1.470 to about 1.575, about 1.480 to about 1.550, and about 1.490 to about 1.525. May be.

[0078] Examples of types or classes of high RI plasticizers are polyadipates (RI of about 1.460 to about 1.485); epoxides such as epoxidized soybean oil (about 1.460 to about 1.480). RI); phthalates and terephthalates (RI of about 1.480 to about 1.540); benzoates and toluates (RI of about 1.480 to about 1.550); and other special plasticizers (about 1.490). Approximately 1.520 RIs), but are not limited to these. Specific examples of suitable RI plasticizers include dipropylene glycol dibenzoate, tripropylene glycol dibenzoate, polypropylene glycol dibenzoate, isodecylbenzoate, 2-ethylhexylbenzoate, diethylene glycol benzoate, butoxyethylbenzoate, butoxyethoxyethylbenzoate, butoxy. Ethoxyethoxyethylbenzoate, propylene glycol dibenzoate, 2,2,4-trimethyl-1,3-pentanediol dibenzoate, 2,2,4-trimethyl-1,3-pentanediol benzoate isobutyrate, 1,3- Butanediol dibenzoate, diethylene glycol di-o-toluate, triethylene glycol di-o-toluate, dipropylene glycol di-o-toluate, 1,2-octyldibenzoate, tri-2-ethylhexyl trimerite, di-2 -Ethylenehexyl terephthalate, bisphenol A bis (2-ethylhexanoate), di (butoxyethyl) terephthalate, di (butoxyethoxyethyl) terephthalate, and mixtures thereof can be mentioned, but not limited to. The high RI plasticizer can be selected from dipropylene glycol dibenzoate, tripropylene glycol dibenzoate, and / or 2,2,4-trimethyl-1,3-pentanediol dibenzoate.

[0079] If the polymer layer or interlayer contains a high RI plasticizer, the plasticizer can be present alone in the layer or blended with one or more additional plasticizers. In addition, one or more other plasticizers may contain a high RI plasticizer, or one or more may be a lower RI plasticizer having a refractive index of less than 1.460. In some embodiments, the lower RI plasticizer may have a refractive index of less than about 1.450, less than about 1.445, or less than about 1.442, selected from the group shown above. can do. When a mixture of two or more types of plasticizers is used as the RI modifier, the mixture may have a refractive index of one or more within the above range.

[0080] When used as an RI modifier in a multilayer interlayer, the high RI plasticizer can be present in different amounts in two or more polymer layers. Similarly, when used as an RI modifier in a resin composition or blended polymer layer, the high RI plasticizer can be partitioned as described above, thereby resulting in a polymer layer with a lower residual hydroxyl content. Alternatively, the domain can be allowed to have a higher amount of high RI plasticizer. In some embodiments, at least about 5 phr, at least about 10 phr, at least about 15 phr, at least about 20 phr, with a high RI plasticizer as the RI modifier on at least one layer, or at least part of the polymer layer or interlayer. It can be included in an amount of at least about 25 phr, at least about 30 phr, at least about 35 phr, and / or about 50 phr or less, about 45 phr or less, or about 40 phr or less. The high RI plasticizer can be present in the polymer layer or interlayer film in an amount in the range of about 5 to about 50 phr, about 10 to about 45 phr, and about 20 to about 40 phr. In some embodiments, the high RI plasticizer is applied to one or more other layers or moieties at least about 50 phr, at least about 55 phr, at least about 60 phr, at least about 65 phr, at least about 70 phr, and / or about 120 phr or less. It may be included in an amount in the range of about 110 phr or less, about 100 phr or less, about 90 phr or less, or about 75 phr or less, or about 50 to about 120 phr, about 55 to about 110 phr, about 60 to about 90 phr, about 65 to about 75 phr. can. These amounts may include any other plasticizer, including those present in the composition having a refractive index of less than 1.460, or may contain only high RI plasticizers.

[0081] When a high RI plasticizer is used as an RI modifier in a multilayer interlayer film, the interlayer film has at least one polymer layer having a first poly (vinyl acetal) resin, and a second poly (vinyl acetal). ) Other polymer layers containing the resin can be included, where the difference between the residual hydroxyl content of the first poly (vinyl acetal) resin and the second poly (vinyl acetal) resin is at least 2% by weight. Is. At least one of the polymer layers contains a high RI plasticizer in an amount sufficient for the absolute value of the difference between the refractive index of the polymer layer and the refractive index of the other polymer layer to be 0.010 or less. Can be done. In some embodiments, the innermost polymer layer may have a higher index of refraction if the interlayer film comprises at least three polymer layers, while in other embodiments, the outer polymer layer. The index of refraction of one or both can be made higher.

[0082] When a high RI plasticizer is included in a polymer layer containing at least one poly (vinyl acetal) resin having a lower residual hydroxyl content, at least a portion of the polymer layer is below 25 ° C., about 20. It can have a glass transition temperature of ° C. or lower, about 15 ° C. or lower, about 10 ° C. or lower, about 5 ° C. or lower, about 0 ° C. or lower, about -5 ° C. or lower, or about -10 ° C. or lower, and this layer is described above. At least about 1.465, at least about 1.470, at least about 1.475, at least about 1.480, at least about 1.485, at least about 1.490, at least about 1.495, at least as measured as described. About 1.500, at least about 1.510, at least about 1.520, at least about 1.525, at least about 1.540, at least about 1.550, at least about 1.575, at least about 1.590, at least about 1 It can have a refractive index of .600, at least about 1.615, at least about 1.625, or at least about 1.650. The plasticizer content of this layer is, in some embodiments, at least about 50 phr, at least about 55 phr, at least about 60 phr, and / or about 120 phr or less, about 110 phr or less, about 90 phr or less, about 85 phr or less, about 80 phr or less. Alternatively, it may be in the range of about 75 phr or less, or about 50 to about 120 phr, about 55 to about 110 phr, about 60 to about 90 phr, or about 60 to about 75 phr.

[0083] When a high RI plasticizer is present in a polymer layer containing a poly (vinyl acetal) resin with a higher residual hydroxyl content, at least a portion of the layer is at least about 26 ° C., at least about 30 ° C. It can have a glass transition temperature of at least about 33 ° C., or at least about 35 ° C., and this layer is at least about 1.470, at least about 1.475, at least about 1.480 as measured as described above. , At least about 1.485, at least about 1.490, at least about 1.495, at least about 1.500, at least about 1.510, at least about 1.520, at least about 1.525, at least about 1.540, at least It can have a refractive index of about 1.550, at least about 1.575, at least about 1.590, at least about 1.600, at least about 1.615, at least about 1.625, or at least about 1.650. The plasticizer content of this layer may be less than 50 phr, less than about 45 phr, less than about 40 phr, less than about 30 phr, or less than about 20 phr, according to some embodiments.

[0084] According to various aspects of the invention, the RI modifier may be one or more layers, or a solid RI additive present in one or more portions of a layer or interlayer film. The term "solid RI additive" as used herein is used to regulate the refractive index of a poly (vinyl acetal) resin, polymer layer, or interlayer film, and is an addition that is solid at 25 ° C. and 1 atmospheric pressure ambient conditions. Refers to an agent. In various embodiments, the solid RI additive is at least about 27 ° C., at least about 30 ° C., at least about 35 ° C., at least about 40 ° C., at least about 45 ° C., at least about 50 ° C., at least about 55 ° C., at least about 60 ° C. It may have a melting point of at least about 75 ° C., at least about 80 ° C., at least about 85 ° C., at least about 90 ° C., at least about 95 ° C., or at least about 100 ° C. When used in resin blends, layers, or interlayer films, solid RI additives are sufficient for the absolute value of the difference between the indices of refraction of the first and second polymer layers to be about 0.010 or less. Can be present in quantity. The difference between the indices of refraction of the first and second polymer layers can be greater than 0.010 when blended into the same polymer layer in the absence of solid RI additives.

[0085] In some embodiments, the solid RI additive may be a high RI solid additive for increasing the index of refraction of at least one polymer layer or interlayer film. The refractive index of the high RI solid additive is at least about 1.460, at least about 1.465, at least about 1.470, at least about 1.475, at least about 1.480, at least as measured as described above. About 1.485, at least about 1.490, at least about 1.495, at least about 1.500, at least about 1.505, at least about 1.510, at least about 1.525, at least about 1.550, at least about 1. .575, or at least about 1.600. In other embodiments, the solid RI additive may be a RI reduced solid additive for reducing the refractive index of at least one resin or polymer layer. RI-lowered solid additives have a refractive index of less than 1.460, about 1.455 or less, about 1.450 or less, about 1.445 or less, or about 1.440 or less as measured as described above. You can do it. Whether higher or lower, the solid RI additive has a refractive index of at least about 0.005, at least about 0.010, at least about 0.050, at least about 0.10, with the index of refraction of the poly (vinyl acetal) resin. And / or may have different refractive indexes of about 0.50 or less, about 0.35 or less, or about 0.20 or less. The difference in refractive index between the solid RI additive and the poly (vinyl acetal) resin is about 0.005 to about 0.50, about 0.010 to about 0.35, or about 0.050 to about 0.35. It may be in the range of.

[0086] In various embodiments, the solid RI additive is in the resin composition or interlayer film, depending on the type of additive and layer or interlayer film specified, at least about 0.5 phr, at least about 1 phr, at least. It can be present in an amount of about 1.5 phr, at least about 2 phr, or at least about 5 phr. Solid RI additives, whether high RI additives or RI lowering additives, are physically mixed or blended with at least one poly (vinyl acetal) resin in the resin composition or layer. A physical solid RI additive that can be included, or it can be reacted with or incorporated into the skeleton of one or more poly (vinyl acetal) resins. It may be a solid RI additive.

[0087] The solid RI additive can be used in combination with one or more low RI plasticizers. Examples of low RI plasticizers are triethylene glycol di (2-ethylhexanoate) (3GEH), triethylene glycol di (2-ethylbutyrate), triethylene glycol diheptanoate, tetraethylene glycol dihepta. Noate, tetraethylene glycol di (2-ethylhexanoate) (4-GEH), dihexyl adipate, dioctyl adipate, hexylcyclohexyl adipate, diisononyl adipate, heptylnonyl adipate, di (butoxyethyl) adipate, and bis (2- (2-Butoxyethoxy) ethyl) adipate, dibutyl sebacate, dioctyl sebacate, and mixtures thereof can be mentioned, but not limited to. The plasticizer can be selected from the group consisting of triethylene glycol di (2-ethylhexanoate) and tetraethylene glycol di (2-ethylhexanoate), or the plasticizer is triethylene glycol di (2-ethylhexanoate). 2-Ethylhexanoate) may be included. The solid RI additive can also be used in combination with one or more of the high RI plasticizers described above.

[0088] If the solid RI additive is a physical solid RI additive, it can be combined with one or more poly (vinyl acetal) resins or layers in the interlayer. In some embodiments, the physical solid RI additive is in at least one layer or interlayer film at least about 1 phr, at least about 2 phr, at least about 3 phr, at least about 5 phr, at least about 8 phr, at least about 10 phr, at least about 10 phr. About 12 phr, at least about 15 phr, at least about 20 phr, and / or about 60 phr or less, about 55 phr or less, about 50 phr or less, about 45 phr or less, about 40 phr or less, about 35 phr or less, about 30 phr or less, about 25 phr or less, about 20 phr or less, Alternatively, it can be present in an amount of about 15 phr or less, or an amount in the range of about 1 to about 60 phr, about 5 to about 50 phr, or about 10 to about 45 phr. Examples of suitable physical solid high RI additives include polyadipates, polystyrenes with a molecular weight of less than 2500, epoxides, phthalates, benzoic acid esters such as inorganic oxides such as zirconium oxide, and combinations thereof. It can be mentioned, but is not limited to these. The physical solid RI lowering additive can be selected from the group consisting of halogenated additives and silicon-containing additives.

[0089] When used in multilayer interlayers, the physical solid RI additive can be present in one of the polymer layers in greater amounts than one or more other layers. The difference between the amount of physical solid RI additive present in one of the polymer layers and the amount of physical solid RI additive present in another layer, for example an adjacent layer, is at least about about. 2 phr, at least about 5 phr, at least about 8 phr, at least about 10 phr, and / or less than about 30 phr, less than about 25 phr, or less than about 20 phr, or this may be about 2 to about 30 phr, about 5 to about 25 phr, or It may be in the range of about 10 to about 20 phr. According to some embodiments, at least one of the layers is at least about 1 phr, at least about 5 phr, at least about 10 phr, at least about 15 phr, and / or about 60 phr or less, about 55 phr or less, about 50 phr or less, about 45 phr or less. The physical solid RI additive can be included, or the physical solid RI additive can be present in an amount in the range of about 1 to about 60 phr, about 10 to about 50 phr, or about 15 to about 45 phr. .. In some embodiments, the physical solid RI additive is at least about 5 phr, at least about 10 phr, at least about 15 phr, at least about 20 phr, and / or about 60 phr or less, about 55 phr or less, about in one or more layers. It can be present in an amount of 50 phr or less, or an amount in the range of about 5 to about 60 phr, about 15 to about 55 phr, or about 20 to about 50 phr.

[0090] When the multilayer interlayer contains three or more polymer layers and the solid RI additive is a solid high RI additive, the inner or core may be in one or more layers, rather than the outer or skin layer. Large amounts of physical solid RI additives can be included. However, when the solid RI additive is a solid RI lowering additive, the outer skin layer can contain a larger amount of the solid RI additive than the inner core layer. The core layer contains at least about 30%, at least about 40%, at least about 50%, at least about 60%, at least about 70%, or at least about 80% of the total amount of physical solid RI additives present in the interlayer. Can be included.

When the solid RI additive is a reactive solid RI additive, it is reacted with at least one poly (vinyl acetal) resin to introduce at least a portion of the additive into the polymer chain. Can be done. The reactive RI additive may be an aromatic additive and, in some embodiments, may include phthalic anhydride and a phenylalkoxysilane such as, for example, diphenyldimethoxysilane.

[0092] In some embodiments, the reactive RI additive is present in one layer of the multilayer interlayer in greater amounts than it is in one or more other layers of the interlayer. Can be done. In some embodiments, it can be excluded from or substantially excluded from one or more polymer layers. For example, if the interlayer film is a multilayer interlayer film containing at least three polymer layers, the inner core layer has at least about 0.5 phr, at least about 1 phr, at least about 1.5 phr, at least about 2 phr, at least about 2 .5 phr, at least about 3 phr, and / or about 50 phr or less, about 30 phr or less, about 20 phr or less, about 15 phr or less, about 12 phr or less, about 10 phr or less, or about 8 phr or less, or about 0.5 to about 20 phr, about 1 One or more reactive solid RI additives can be included in an amount ranging from ~ about 12 phr, or about 2 ~ about 8 phr. One or more outer skin layers may contain reactive solid RI additives of about 10 phr or less, about 5 phr or less, about 2 phr or less, about 1 phr or less, or about 0.5 phr or less. The core layer can contain at least about 65%, at least about 75%, at least about 85%, at least about 95%, or at least about 99% of the total amount of reactive RI additives present in the interlayer. ..

[0093] When a solid RI additive is used as an RI modifier in a multilayer interlayer, the interlayer has at least one polymer layer having a first poly (vinyl acetal) resin and a second poly (vinyl acetal) resin. ) Other polymer layers containing the resin can be included, where the difference between the residual hydroxyl content of the first poly (vinyl acetal) resin and the second poly (vinyl acetal) resin is at least 2% by weight. be. An amount of high RI additive on at least one of the polymer layers sufficient for the absolute value of the difference between the refractive index of the first polymer layer and the refractive index of the second polymer layer to be 0.010 or less. Can be included in. In some embodiments where the interlayer film comprises at least three polymer layers, the innermost polymer layer may have a higher index of refraction, while in other embodiments one or more of the outer polymer layers. Both refractive indexes can be made higher.

[0094] When solid RI additives are included in a polymer layer containing a poly (vinyl acetal) resin with a lower residual hydroxyl content, the polymer layers are measured as described above, respectively, 25. Glass transition temperature of ° C. or lower, about 20 ° C. or lower, about 15 ° C. or lower, about 10 ° C. or lower, about 5 ° C. or lower, about 0 ° C. or lower, about -5 ° C. or lower, or about -10 ° C. or lower, and at least about 1. 465, at least about 1.470, at least about 1.475, at least about 1.480, at least about 1.485, at least about 1.495, at least about 1.500, at least about 1.510, at least about 1.520, At least about 1.525, at least about 1.540, at least about 1.550, at least about 1.575, at least about 1.590, at least about 1.600, at least about 1.615, at least about 1.625, or at least It can have a refractive index of about 1.650. The plasticizer content of this layer is, in some embodiments, at least about 50 phr, at least about 55 phr, at least about 60 phr, at least about 65 phr, and / or about 120 phr or less, about 110 phr or less, about 90 phr or less, about 85 phr or less. It may be in the range of about 80 phr or less, or about 75 phr or less, or about 50 to about 120 phr, about 55 to about 110 phr, about 60 to about 90 phr, about 65 to about 75 phr.

[0095] When a solid RI additive is present in a polymer layer containing a poly (vinyl acetal) resin with a higher residual hydroxyl content, the layer is at least about 26 ° C, at least about 30 ° C, at least about 33. It can have a glass transition temperature of ° C., or at least about 35 ° C. In some embodiments, the layer is at least about 1.470, at least about 1.475, at least about 1.480, at least about 1.485, at least about 1.490, at least about 1.500, at least about 1. .510, at least about 1.520, at least about 1.525, at least about 1.540, at least about 1.550, at least about 1.575, at least about 1.590, at least about 1.600, at least about 1.615 , Can have a refractive index of at least about 1.625, or at least about 1.650. The plasticizer content of this layer may be less than 50 phr, less than about 45 phr, less than about 40 phr, less than about 30 phr, or less than about 20 phr, according to some embodiments.

[0096] According to some embodiments, the index of refraction of the interlayer film is higher than 1.475, as measured above, at least about 1.480, at least about 1.490, at least about 1. 500, at least about 1.510, at least about 1.520, at least about 1.530, at least about 1.540, at least about 1.550, at least about 1.560, at least about 1.570, at least about 1.580, At least about 1.590, at least about 1.600, at least about 1.610, at least about 1.620, at least about 1.630, at least about 1.640, at least about 1.650, at least about 1.660, or at least It can be about 1.670. The interlayer film may contain one or more RI modifiers described herein, or one or more other RI modifiers not specifically mentioned. The interlayer can be a single layer (or a monolith interlayer), or it can include two or more layers adjacent to each other as discussed herein.

[0097] Resin compositions, layers, and interlayer films prepared by incorporating at least two types of poly (vinyl acetal) resins and RI modifiers according to various aspects of the present invention are such as impact resistance and sound insulation performance. It is possible to exhibit improved optical characteristics without sacrificing other characteristics. As discussed above, the same blend of the same resin prepared without an RI modifier due to differences in the properties or composition of the resin, such as residual hydroxyl content, residual acetate content, or aldehyde residues, It may provide compositions, layers, and interlayer films with reduced optical performance.

[0098] Clarity is a parameter used to indicate the optical performance of the compositions, layers, and interlayer films described herein and can be determined by measuring cloudiness or%. .. The degree of cloudiness is a quantification of the light scattered by the sample with respect to the incident light. In some embodiments, the resin blends, layers, and interlayers described herein are less than 5% as measured at a 2 ° observation angle using light source C according to ASTM-D1003-13-Procedure B. , Less than about 4%, less than about 3%, less than about 2%, less than about 1%, or less than about 0.5% cloudiness. The tests were conducted using spectrophotometers such as the Hunterlab UltraScan XE instrument (commercially available from Hunter Associates, Reston, VA), clear glass, each with a thickness of 2.3 mm (Pittsburgh Glass Works, Pennsylvania). For a polymer sample with a thickness of 0.76 mm laminated between two sheets (commercially available from).

[0099] Further, the polymer layers and interlayers described herein can have a color spot value of 3 or less, 2 or less, or 1 or less. Color spots are another indicator of optical quality detected as texture or graininess. Color spots are visual defects when their levels are excessively high or excessively intense, thereby resulting in an unfavorable appearance. Color spots represent a shadow graph projection of the test laminate, with a color spot value in the range 1-4 (1 representing a low color spot (ie, a small number of confusions)) and 4 being a high color spot (ie, a large number). Evaluated and categorized by alternating qualitative comparisons with a set of standard laminated shadow graphs representing a series or scale of). High color spots are generally considered unfavorable, especially in automotive and architectural applications. In some cases, model laminates with a single layer interlayer with zero color spots (no color spots) have a color spot grade lower than the scale of the reference set, such as lower than grade 1. Facilitates evaluation in test laminates. A test laminate showing a shadow graph projection similar to that of a zero-spot stack is evaluated to have a zero-spot grade. The test laminate is prepared using two sheets of clear glass (commercially available from Pittsburgh Glass Works, Pennsylvania), each with a thickness of 2.3 mm, and an interlayer film. The interlayer film usually has a random surface roughness of about 35-40 microns: R _z , and a thickness of 0.76 to 0.86 mm.

The color spot value given here was determined using a Clear Mottle Analyzer (CMA) including a xenon arc lamp, a sample holder, a projection screen, and a digital camera. The camera was configured to project a shadow graph of the laminated sample onto a screen using a xenon arc lamp and record the resulting shadow graph image. Next, the image was digitally analyzed using computer imaging software, and the color spots of the sample were determined by comparing with the image of the standard sample recorded in advance. A method for determining color spots using CMA is described in detail in US Patent Application Publication US-2012-0133764.

[0101] Another parameter used to determine optical performance is transparency or visible transmittance (% T _vis ), which uses a spectrophotometer such as HunterLab UltraScan EX according to ASTM-D1003 procedure B. It is measured at an observation angle of 2 ° using the light source C. The values given here are obtained by analyzing glass laminate samples with an interlayer thickness of approximately 0.76 mm and a thickness of 2.3 mm clear glass (commercially available from Pittsburgh Glass Works, Pennsylvania). Obtained. In some embodiments, the polymer layers and interlayers of the invention are at least about 70%, at least about 75%, at least about 80%, at least about 81%, at least about 82%, at least about 83%, at least about 84. %, At least about 85%, at least about 85.5%, at least about 86%, at least about 86.5%, at least about 87%, at least about 87.5%, at least about 88%, or at least about 88.5% Can have a visible transmittance (%) of. More specifically, the polymer layers and interlayer films of the present invention are higher than 85% for interlayer films containing only additives such as ACA, UV stabilizers, and antioxidants, or the pigments, IR absorbers or the above-mentioned pigments, IR absorbers or It has a _{% T-vis} higher than 80% for interlayer films containing additional additives such as blockers. Polymer interlayers containing high levels of pigments and / or dyes, such as raw material colored or colored polymer interlayers, can have _{lower% T vis values as desired.}

[0102] In addition to exhibiting one or more optical properties within the above range, the polymer layers and interlayer films described herein can also exhibit sound insulation properties within the desired range. In some embodiments, as discussed above, at least a portion of the polymer layer or interlayer film is 25 ° C. or lower, about 20 ° C. or lower, about 15 ° C. or lower, about 10 ° C. or lower, about 5 ° C. or lower, about. It may have a glass transition temperature of 0 ° C. or lower, about −5 ° C. or lower, or about −10 ° C. or lower, which can promote the sound insulation performance of the layer or the interlayer film. At the same time, at least a portion of the layer or interlayer may have a glass transition temperature of at least about 26 ° C, at least about 30 ° C, and at least about 35 ° C, which can promote impact resistance and strength. ..

[0103] In some embodiments, the polymer layer or interlayer film according to the invention can have a value of at least about 0.70 tan δ. tan δ is the ratio of the loss modulus (G ″) (Pascal) to the storage modulus (G') (Pascal) of the sample measured by dynamic mechanical thermal analysis (DMTA). DMTA is a frequency of 1 Hz. The peak value of the G "/ G'curve at the glass transition temperature is the value of tan δ. The polymer layers or interlayers described herein according to various aspects are at least about 1.0, at least about 1.05, at least about 1.10, at least about 1.25, at least about 1.50, at least about 1. It can have 75, at least about 2.0, or at least about 2.25 tan δ.

[0104] Further, the polymer layer and the interlayer are at least about 0.10, at least about 0.15, at least about 0.17, at least about 0.20, at least about 0.25, at least about 0.27, at least about 0.27. It can have a damping loss factor, or loss factor of about 0.30, at least about 0.33, or at least about 0.35. The loss factor is measured by mechanical impedance measurement as described in ISO standard 16940. A polymer sample is laminated between two sheets of clear glass, each having a thickness of 2.3 mm, and prepared to have a width of 25 mm and a length of 300 mm. The laminated sample is then excited at the center point using a vibrating shaker commercially available from Bruel and Kjaer (Naerum, Netherlands) and the bar is excited using an impedance head (Bruel and Kjaer). And measure the force required to vibrate and the speed of vibration. The resulting transfer function is recorded in the National Instrument data acquisition and analysis system and the loss factor in the first vibration mode is calculated using the half-power method. In some embodiments, when the RI modifier is a high RI plasticizer, the layer or interlayer is higher than 0.25, higher than 0.27, higher than 0.30, or 0. The layer or interlayer can have a loss coefficient greater than 35, while in other embodiments, the layer or interlayer is 20 ° C., where the RI modifier is a solid RI additive or a residue of at least one high RI aldehyde. Can have a loss coefficient of at least about 0.10, at least about 0.15, at least about 0.20, at least about 0.25, or at least about 0.30.

[0105] Similar to a resin blend of two separate resins, a first poly (vinyl acetal) resin and a second poly (vinyl acetal) resin, blending two or more separate polymer layers or interlayers It is often possible to obtain novel one or more polymer layers or one or more interlayer films with unexpected properties and performance attributes. For example, a polymer layer or interlayer with a lower residual hydroxyl content and a lower glass transition temperature can be blended with another polymer layer or interlayer with a higher residual hydroxyl content and a higher glass transition temperature to lower the glass. A soft domain with a transition temperature (which improves its sound insulation performance) and a hard domain with a higher glass transition temperature (which provides improved workability, strength, and impact resistance to the polymer layer or interlayer film). ) Can be provided as a novel polymer layer or interlayer film. Other examples include blending a single sheet interlayer film with a multilayer interlayer film, blending two multilayer interlayer films, or blending one multilayer interlayer film into a polymer layer of another multilayer interlayer film. Can be mentioned. In essence, the effect obtained by blending the two materials can also be achieved by blending two or more resins, plasticizers, and other additives according to the contents of the material. The "blend resin material" or "blend material" used herein means a resin composition, a polymer layer, or an intermediate to be blended in another resin composition, a polymer layer, or an interlayer film. Refers to the membrane. When blending two polymer layers or two interlayer films, at least one of the two materials to be blended may include the polymer layer or interlayer film of the present invention. In other embodiments, both materials can include the polymer layer or interlayer film of the invention.

[0106] According to some embodiments, at least a portion of the resin composition, layer, or interlayer film described herein may include another resin, layer, or interlayer film. In some embodiments, at least about 0.5%, at least about 1%, at least about 5%, at least about 10%, at least about 15%, at least about about the total amount of resin in the composition, layer, or interlayer film. 20%, at least about 25%, at least about 30%, or at least about 50% can be derived from the blended resin material.

[0107] Often, the type and / or amount of resin and plasticizer in the blended resin material is substantially different from the type and / or amount of resin or plasticizer produced in which the blended resin material is added. In some cases, the clarity or cloudiness of the resulting resin composition, layer, or interlayer film containing the blended resin material can adversely affect the optical performance required. According to some aspects of the invention, polymer layers and interlayers containing higher levels of blended resin material can be made by using one or more of the RI modifiers discussed above.

[0108] The resins described herein without reducing or increasing the clarity of the final composition, layer, or interlayer film when the RI modifier comprises a high RI plasticizer. A larger amount of blended resin material can be added to the process of making the composition, layer, or interlayer film. In some embodiments, the composition comprising the blend material may include a first poly (vinyl acetal) resin and a second poly (vinyl acetal) resin, wherein one of the resins is of the other resin. It has a residual hydroxyl content that may be at least 2% by weight lower than the residual hydroxyl content. Such compositions may further comprise at least one high RI plasticizer having a refractive index of 1.460, in some embodiments present in the composition, layer, or interlayer film. More than 3% of the total amount of the first and second poly (vinyl acetal) resins can be derived from the blend composition, layer, or interlayer film. Compositions containing more than 0.5% by weight of blended resin materials, regardless of the difference in residual hydroxyl content of the first and second poly (vinyl acetal) resins, are about 5 or less, about 4 or less, about 3 or less, It can have a cloudiness of about 2 or less, or about 1 or less, or about 0.5 or less.

[0109] The high RI plasticizer used as the RI adjuster together with the blended resin composition may have a refractive index within the range of 1 or more described above. The high RI plasticizer can be added with the blend material during the production of the composition, layer, or interlayer and / or at least a portion of the high RI plasticizer is present in the blended resin material added to the process. Can be made to. Further, one or more other plasticizers, such as those having a refractive index of less than about 1.450, less than about 1.445, or less than about 1.442 as measured as described above, are further blended. It can also be present in the resin material and / or in the resin composition, layer, or interlayer film produced. In some embodiments, one or more additional high RI plasticizers may also be present in the blending material and / or in the resin composition, layer, or interlayer film in which the material is blended. ..

[0110] Resin compositions containing the blended resin materials described above can be used to form layers and interlayer films according to various aspects of the invention. For example, a resin composition containing a blended resin material can be used to form a single monolithic interlayer film, or it can be used to form one or more layers of a multilayer interlayer film. When used in various layers and interlayers, additional plasticizers should be added to allow the total amount of the plasticizer present in the polymer layer or interlayer to be within the range described above. Can be done. Similarly, the glass transition temperature and refractive index of the polymer layer and the interlayer film formed from the composition containing the blended resin material can be set within the above-mentioned ranges. Further, polymer layers and interlayer films formed from compositions containing blended materials can also exhibit the sound insulation properties described above and can be included in any of the applications described below.

[0111] According to some embodiments, at least a portion of the resin composition, layer, or interlayer film described herein is one or more recycled resins, such as a recycled layer or interlayer film. Materials can be included. The term "recycled" as used herein means that it is removed from the production line and then returned. Often, the use of recycled materials adversely affects the optical performance of the final composition, layer, or interlayer film as determined by clarity or haze due to the different composition and properties of the blended or mixed materials. there is a possibility. However, in some embodiments, at least one type of recycled resin material is used in the layers or interlayer films described herein, while still exhibiting optical and / or sound insulation properties equivalent to those described herein. Can be included. The type and / or amount of the recycled resin material may be in the range of one or more described above, and the layer or interlayer film may further contain at least one RI modifier. Further, the polymer layer and the interlayer film containing the recycled resin material can also have optical and / or sound insulation performance within one or more ranges described below.

[0112] The resin compositions, layers, and interlayer films described above can be produced according to any suitable method. In various embodiments, the method of producing these compositions, layers, and interlayer films is provided with two or more poly (vinyl acetal) resins and at least one resin is an RI modifier and, in some cases, at least one. It can include blending with one type of plasticizer or other additive to form a blended composition, and forming a layer from the blended composition.

[0113] In some embodiments, the resin given in the first step of the method may be in the form of one or more poly (vinyl acetal) resins, while in other embodiments one or more. A resin precursor can also be given. In some embodiments, when physically blending two or more poly (vinyl acetal) resins, blending the two resins can include melt blending, which is at least about 140. It can be carried out at a temperature of at least about 150 ° C., at least about 180 ° C., at least about 200 ° C., and at least about 250 ° C. In another embodiment, if the given poly (vinyl acetal) resin component contains a resin precursor, the blending step involves reacting two or more aldehydes with polyvinyl alcohol to a single having two or more aldehyde groups. Can include giving a poly (vinyl acetal) resin. Further, part of the blending step can include blending one or more of the resins with at least one of the plasticizers and / or one or more of the RI modifiers described above.

The resulting blended resin can then be molded into one or more polymer layers according to any suitable method. Typical methods for forming the polymer layer and interlayer film include, but are not limited to, solution casting, compression molding, injection molding, melt extrusion, melt blowing, and combinations thereof. Multilayer interlayers containing two or more polymer layers are also available, for example, in coextrusions, blown films, melt blows, immersion coatings, solution coatings, blade coatings, paddle coatings, air knife coatings, printing, powder coatings, spray coatings, and combinations thereof. It can also be produced according to any suitable method such as. In various aspects of the invention, the layer or interlayer can be formed by extrusion or coextrusion. In the extrusion process, at least one additive, such as one or more thermoplastic polymers, plasticizers, and possibly one or more RI modifiers described above, is premixed and fed into the extruder. can do. Other additives such as ACA, colorants, and UV inhibitors, which may be in liquid, powder, or pellet form, can also be used in the thermoplastic polymer or plasticizer prior to introduction into the extruder. Can be mixed. These additives are introduced into the polymer resin and into the polymer sheet obtained by expanding interpretation, thereby causing some properties of the polymer layer or interlayer film, and its in the final multilayer glass panel or other final product. Performance can be improved.

[0115] In various embodiments, the thickness or gauge of the layer or interlayer is at least about 10 mils, at least about 15 mils, at least about 20 mils, and / or about 100 mils or less, about 90 mils or less, about 60. It may be mils or less, about 50 mils or less, or about 35 mils or less, or it may be in the range of about 10 to about 100 mils, about 15 to about 60 mils, or about 20 to about 35 mils. The thickness of the polymer layer or interlayer film in millimeters is at least about 0.25 mm, at least about 0.38 mm, at least about 0.51 mm, and / or about 2.54 mm or less, about 2.29 mm or less, about 1.52 mm. Below, or about 0.89 mm or less, or in the range of about 0.25 to about 2.54 mm, about 0.38 to about 1.52 mm, or about 0.51 to about 0.89 mm. In some embodiments, the polymer layer or interlayer film comprises a flat polymer layer having substantially the same thickness along the length or longest dimension and / or width or second longest dimension of the sheet. On the other hand, in other embodiments, for example, one or more layers of the multilayer interlayer film may be tapered or given a wedge-shaped profile so that the thickness of the interlayer film is the length and / or width of the sheet. Can be varied along so that one edge of the layer or interlayer film has a greater thickness than the other. When the interlayer film is a multilayer interlayer film, at least one, at least two, or at least three layers of the interlayer film can include at least one tapered area. If the interlayer film is a monolithic interlayer film, the polymer sheet can be flattened or can include at least one tapered area. Tapered interlayers may be useful in head-up display (HUD) panels, for example in automotive and aircraft applications.

[0116] With reference to FIGS. 1-8, some aspects of the tapered interlayer according to the present invention are given. FIG. 1 is a cross-sectional view of a typical tapered interlayer film including tapered areas of various thicknesses. As shown in FIG. 1, the tapered area has a minimum thickness measured at the first boundary of the tapered area: T _min , and a maximum thickness measured at the second boundary of the tapered area. : _Has T max. In some embodiments, T _min is at least about 0.25 mm (mm), at least about 0.40 mm, or at least about 0.60 mm, and / or 1.2 mm or less, about 1.1 mm or less, or about. It may be 1.0 mm or less. Further, T _min may be in the range of 0.25 to 1.2 mm, 0.4 to 1.1 mm, or 0.60 to 1.0 mm. In some embodiments, the T _max is at least about 0.38 mm, at least about 0.53 mm, or at least about 0.76 mm, and / or 2.2 mm or less, about 2.1 mm or less, or about 2.0 mm or less. May be. Further, the T _max may be in the range of 0.38 to 2.2 mm, 0.53 to 2.1 mm, or 0.76 to 2.0 mm. In some embodiments, _{the difference between T max} and T _min is at least about 0.13 mm, at least about 0.15 mm, at least about 0.2 mm, at least about 0.25 mm, at least about 0.3 mm, at least about. 0.35 mm, at least about 0.4 mm and / or 1.2 mm or less, about 0.9 mm or less, about 0.85 mm or less, about 0.8 mm or less, about 0.75 mm or less, about 0.7 mm or less, about 0 It may be .65 mm or less, or about 0.6 mm or less. Further, _{the difference between T max} and T _min may be in the range of 0.13 to 1.2 mm, 0.25 to 0.75 mm, or 0.4 to 0.6 mm. In some embodiments, the distance between the first and second boundaries of the tapered area (ie, the width of the tapered area) is at least about 5 cm (cm), at least about 10 cm, at least about 15 cm. , At least about 20 cm, or at least about 30 cm, and / or about 200 cm or less, about 150 cm or less, about 125 cm or less, about 100 cm or less, or about 75 cm or less. Further, the width of the tapered area may range from 5 to 200 cm, 15 to 125 cm, or 30 to 75 cm.

[0117] As shown in FIG. 1, the tapered interlayer includes contralateral first and second outer ends. In some embodiments, the distance between the first and second outer ends (ie, the width of the interlayer) is at least about 20 cm, at least about 40 cm, or at least about 60 cm, and / or about 400 cm or less, about. It may be 200 cm or less, or about 100 cm or less. Further, the width of the interlayer film may be in the range of 20 to 400 cm, 40 to 200 cm, or 60 to 100 cm. In the embodiment shown in FIG. 1, the first and second boundaries of the tapered area are inwardly separated from the first and second outer ends of the interlayer film. In such an embodiment, only a part of the interlayer film is tapered. If the tapered area forms only part of the interlayer, the ratio of the width of the interlayer to the width of the tapered area is at least about 0.05: 1, at least about 0.1 :. 1. At least about 0.2: 1, at least about 0.3: 1, at least about 0.4: 1, at least about 0.5: 1, at least about 0.6: 1, or at least about 0.7: 1. And / or about 1: 1 or less, about 0.95: 1 or less, about 0.9: 1 or less, about 0.8: 1 or less, or about 0.7: 1 or less. Further, the ratio of the width of the interlayer to the width of the tapered area may be in the range of 0.05: 1 to 1: 1 or 0.3: 1 to 0.9: 1. In another aspect discussed below, the entire interlayer film is tapered. If the entire interlayer film is tapered, the width of the tapered area is equal to the width of the interlayer film, and the first and second boundaries of the tapered area are at the first and second ends, respectively. To position.

[0118] As shown in FIG. 1, there are two tapered areas of the interlayer film, one in which the boundary between the first and second tapered areas intersects the first (upper) surface of the interlayer film. A first reference line extending through a point and a second reference line extending through two points where the boundary between the first and second tapered areas intersects the second (lower) surface of the interlayer film. It has a wedge angle defined as the angle formed between and. In some embodiments, the wedge angle of the tapered area is at least about 0.13 milliradian (mrad), at least about 0.15 mrad, at least about 0.2 mrad, at least about 0.25 mrad, at least about 0.3 mrad, At least about 0.35 mrad, at least about 0.4 mrad, and / or about 1.2 mrad or less, about 1.0 mrad or less, about 0.9 mrad or less, about 0.85 mrad or less, about 0.8 mrad or less, about 0.75 mrad or less , About 0.7 mrad or less, about 0.65 mrad or less, about 0.6 mrad or less, about 0.55 mrad or less, about 0.5 mrad or less, or about 0.45 mrad or less. Further, the wedge angle of the tapered area is 0.13 to 1.2 mrad, 0.2 to 0.8 mrad, 0.25 to 0.75 mrad, 0.3 to 0.6 mrad, or 0.4 to 0. It may be in the range of 55 mrad.

[0119] If the first and second surfaces of the tapered area are planar, respectively, then the wedge angles of the tapered area are simply the first (top) surface and the second (bottom). The angle between the surfaces. However, as discussed in more detail below, in some embodiments, the tapered area comprises at least one variable angle area with a curvilinear thickness profile and a continuously changing wedge angle. You can go out. Further, in some embodiments, the tapered area may include two or more constant angle areas, where the constant angle areas each have a linear thickness profile, but at a constant angle. At least two of the areas of have different wedge angles.

[0120] FIGS. 2-7 show various tapered interlayer films constructed according to a plurality of aspects of the present invention. FIG. 2 shows an interlayer film 20 including a tapered area 22 that completely extends from the first end portion 24a of the interlayer film 20 to the second end portion 24b of the interlayer film 20. In this structure, the first and second boundaries of the tapered area are located at the first and second end portions 24a, b of the interlayer film. The entire tapered area 22 of the interlayer film 20 shown in FIG. 2 is simply at an angle formed between the first (upper) planar and second (lower) planar surfaces of the interlayer film 20. It has a certain wedge angle: θ.

[0121] FIG. 3 shows an interlayer film 30 including a tapered area 32 and a horizontal end area 33. The first boundary 35a of the tapered area 32 is located at the first end 34a of the interlayer film 30, while the second boundary 35b of the tapered area 32 is an end horizontal to the tapered area 32. It is located at the intersection of the sections 33. The tapered area 32 includes a constant angle area 36 and a variable angle area 37. The constant angle area 36 has a linear thickness profile and a constant wedge angle: θ _c , while the variable angle area 37 has a curved thickness profile and a continuously changing wedge angle. The starting wedge angle of _{the variable angle area 37 is equal to a constant wedge angle: θ c,} and the ending wedge angle of the variable angle area 37 is zero. The interlayer film 30 shown in FIG. 3 has a constant wedge angle: θ _c, which is larger than the overall wedge angle of the entire tapered area 32.

[0122] FIG. 4 shows an interlayer film 40 including a tapered area 42 located between the first and second horizontal end areas 43a, b. The first boundary 45a of the tapered area 42 is located at the intersection of the tapered area 42 and the first horizontal end area 43a, while the second boundary 45b of the tapered area 42 is. It is located at the intersection of the tapered area 42 and the second horizontal end area 43b. The tapered area 42 includes a constant angle area 46 located between the first and second variable angle areas 47a, b. The first variable angle zone 47a forms a transition zone between the first horizontal end zone 43a and the constant angle zone 46. The second variable angle zone 47b forms a transition zone between the second horizontal end zone 43b and the constant angle zone 46. The constant angle zone 46 has a linear thickness profile and a constant wedge angle: θ _c , while the first and second variable angle zones 47a, b have a curvilinear thickness profile and continuously. Has a changing wedge angle. The starting wedge angle of the first variation angle area 47a is equal to 0 and the ending wedge angle of the first variation angle area 47b is equal to a _{constant wedge angle: θ c.} The starting wedge angle of _{the second variation angle area 47b is equal to the constant wedge angle: θ c} , and the ending wedge angle of the second variation angle area 47b is zero. The interlayer film 40 shown in FIG. 4 has a constant wedge angle: θ _c, which is larger than the overall wedge angle of the entire tapered area 42.

[0123] FIG. 5 shows an interlayer film 50 including a tapered area 52 located between the first and second horizontal end areas 53a, b. The tapered area 52 of the interlayer film 50 does not include a constant angle area. On the contrary, the entire tapered area 52 of the interlayer film 50 is a variable angle area with a curved thickness profile and a continuously changing wedge angle. As described above, the overall wedge angle of the tapered area 52: θ is such that the first and second boundaries 55a, b of the tapered area 52 are the first (upper) surface of the interlayer film 50. The first reference line "A" extending through the two points intersecting with the first and second boundaries 55a and b of the tapered area 52 intersect the second (lower) surface of the interlayer film 50 2 It is measured as the angle between the second reference line "B" extending through the two points. However, within the tapered area 52, the curved thickness profile has an infinite number of wedge angles that may be greater than, less than, or equal to the overall wedge angle of the entire tapered area 52: θ. give.

[0124] FIG. 6 shows an interlayer film 60 that does not include a horizontal end. On the contrary, the tapered area 62 of the interlayer film 60 forms the entire interlayer film 60. Thus, the first and second boundaries 65a, b of the tapered area 60 are located at the first and second end portions 64a, b of the interlayer film 60. The tapered area 62 of the interlayer film 60 includes first, second, and third constant angle areas 46a, b, c separated by first and second variable angle areas 47a, b. .. The first, second, and third constant angle areas 46a, b, and c each have a linear thickness profile, each of which has its own unique first, second, and third constant. Wedge angle: _Has θ c1, θ _c2 , and θ _c3 . The first variable angle zone 47a functions as a transition zone between the first and second constant angle zones 46a, b. The second variable angle zone 47b functions as a transition zone between the second and third constant angle zones 46b, c. As discussed above, the overall rust angle of the tapered area 62: θ is measured as the angle between the first reference line “A” and the second reference line “B”. The first constant wedge angle: θ _c1 is smaller than the overall wedge angle of the tapered area 62: θ. The second constant wedge angle: θ _c2 is greater than the overall wedge angle of the tapered area 62: θ. The third constant wedge angle: θ _c3 is smaller than the overall wedge angle of the tapered area 62: θ. The wedge angle of the first variable angle area 47a continuously increases _{from the first constant wedge angle: θ c1} to the second constant wedge angle: θ _c2. The wedge angle of the second variable angle area 47b continuously decreases _{from the second constant wedge angle: θ c2} to the third wedge angle: θ _c3.

[0125] FIG. 7 shows an interlayer film 70 including a tapered area 72 located between the first and second horizontal end areas 73a, b. The first and second boundaries 75a and b of the tapered area 72 are inwardly separated from the first and second outer ends 74a and b of the interlayer film 70. The tapered areas 72 of the interlayer film 70 are the first, second, third, and fourth variable angle areas 77a, b, c, d, and the first, second, and third constant angles. Includes areas 76a, b, c. The first variable angle zone 77a functions as a transition zone between the first horizontal end zone 73a and the first constant angle zone 76a. The second variable angle zone 77b functions as a transition zone between the first constant angle zone 76a and the second constant angle zone 76b. The third variable angle zone 77c functions as a transition zone between the second constant angle zone 76b and the third constant angle zone 76c. The fourth variable angle zone 77d serves as a transition zone between the third constant angle zone 76c and the second horizontal end zone 73b. The first, second, and third constant angle areas 76a, b, and c each have a linear thickness profile, each of which has its own unique first, second, and third constant. Wedge angle: _Has θ c1, θ _c2 , and θ _c3 . As discussed above, the first, second, third, and fourth swing angle zones 77a, b, c, d are wedge angles of a constant angle zone on one side of the swing angle zone 77. Has a wedge angle that continuously transitions from to the wedge angle of the constant angle area on the other side of the variable angle area 77.

[0126] As discussed above, the tapered interlayers each have a width smaller than the overall width of the entire tapered area, and each has an overall wedge angle of the entire tapered area. It may include one or more constant angle tapered areas with the same or different wedge angles. For example, the tapered area may include one, two, three, four, five, or more constant angle tapered areas. When using multiple constant-angle tapered areas, the constant-angle tapered areas are placed on top of each other by a variable-angle tapered area that acts to transition between adjacent constant-angle tapered areas. May be separated from.

[0127] In some embodiments, the width of each tapered area at a given angle is at least about 2 cm, at least about 5 cm, at least about 10 cm, at least about 15 cm, or at least about 20 cm, and / or about 150 cm or less. , About 100 cm or less, or about 50 cm or less. In some embodiments, the ratio of the width of each tapered area to the overall width of the entire tapered area is at least about 0.1: 1 and at least about 0.2: 1. , At least about 0.3: 1, or at least about 0.4: 1, and / or about 0.9: 1 or less, about 0.8: 1 or less, about 0.7: 1 or less, about 0.6: It may be 1 or less, or about 0.5: 1 or less.

[0128] In some embodiments, the wedge angle of each tapered area at a certain angle is at least about 0.13 mrad, at least about 0.15 mrad, at least about 0.2 mrad, at least about 0.25 mrad, at least about. 0.3 mrad, at least about 0.35 mrad, or at least about 0.4 mrad, and / or about 1.2 mrad or less, about 1.0 mrad or less, about 0.9 mrad or less, about 0.85 mrad or less, about 0.8 mrad or less, It may be about 0.75 mrad or less, about 0.7 mrad or less, about 0.65 mrad or less, or about 0.6 mrad or less. Further, the wedge angle of each constant angle tapered area may be in the range of 0.13 to 1.2 mrad, 0.25 to 0.75 mrad, or 0.4 to 0.6 mrad. In some embodiments, the wedge angle of at least one constant angle tapered area is at least about 0.01 mrad, at least about 0.05 mrad, and at least about 0 than the overall wedge angle of the entire tapered area. .1 mrad, at least about 0.2 mrad, at least about 0.3 mrad, or at least about 0.4 mrad greater. In some embodiments, the wedge angle of at least one constant angle tapered area is at least about 0.01 mrad, at least about 0.05 mrad, and at least about 0 than the overall wedge angle of the entire tapered area. .1 mrad, at least about 0.2 mrad, at least about 0.3 mrad, or at least about 0.4 mrad smaller. In some embodiments, the wedge angle of at least one constant angle tapered area is about 0.4 mrad or less, about 0.3 mrad or less, about 0. It is 2 mrad or less, about 0.1 mrad or less, about 0.05 mrad or less, or about 0.01 mrad or less larger. In some embodiments, the wedge angle of at least one constant angle tapered area is about 0.4 mrad or less, about 0.3 mrad or less, about 0. 2 mrad or less, about 0.1 mrad or less, about 0.05 mrad or less, or about 0.01 mrad or less smaller.

[0129] FIGS. 8a and 8b show an interlayer film 80 having a thickness profile similar to that of the interlayer film 30 of FIG. The interlayer film 80 of FIGS. 8a and 8b is configured by fixing the interlayer film between two sheets of glass for use in the windshield of a vehicle. As shown in FIG. 8a, the first end 84a of the interlayer 80 can be placed on the bottom of the windshield, while the second end 84b of the interlayer 80 can be placed on the top of the windshield. Can be done. The tapered area 82 of the interlayer film 80 is located within the area of the windshield where the heads-up display is located. The tapered area 82 of the interlayer film 80 includes a constant angle area 86 and a variable angle area 87. As shown in FIG. 8a, in some embodiments, the tapered area 82 places the interlayer film 80 as a whole between the first side edge portion 88a and the second side end portion 88b of the interlayer film 80. Stretch across. FIG. 8b shows the thickness profile of the interlayer film 80 between the bottom of the windshield and the top of the windshield, similar to FIG.

[0130] Although not shown in the drawings, it should be understood that in some embodiments, the tapered interlayer may be a multilayer interlayer. If the tapered interlayer contains multiple individual layers, all of the individual layers may be tapered, some of the individual layers may be tapered, or one of the individual layers. Only may be tapered. Moreover, in some embodiments, the glass transition temperatures of the individual layers may differ from each other. For example, in one embodiment, the interlayer comprises a tapered central layer having a lower glass transition temperature than the two tapered outer layers of the interlayer, in this case one or both glass transitions of the outer layer. The temperature is at least 10 ° C., at least about 20 ° C., at least about 30 ° C., at least about 40 ° C., or at least about 50 ° C. higher than the glass transition temperature of the central layer.

[0131] In some embodiments, the polymer layer or interlayer is provided with a flat polymer layer having substantially the same thickness along the length or longest dimension and / or width or second longest dimension of the sheet. It can be included, while in other embodiments, for example, one or more layers of the multilayer interlayer film are wedge-shaped or given a wedge-shaped profile so that the thickness of the interlayer film is the length of the sheet and / Or can vary along the width so that one end of the layer or interlayer film has a greater thickness than the other. When the interlayer film is a multilayer interlayer film, at least one, at least two, or at least three of the plurality of layers of the interlayer film can be wedge-shaped. When the interlayer film is a monolith type interlayer film, the polymer sheet can be flat or wedge-shaped. Wedge-shaped interlayer films may be useful in head-up display (HUD) panels, for example in automotive and aircraft applications.

[0132] The resin composition, layer, and interlayer film according to the plurality of aspects of the present invention can be used in a multilayer panel containing a polymer layer or an interlayer film and at least one hard substrate. In some embodiments, the multilayer panel comprises a pair of hard substrates with a resin interlayer placed between them. The total thickness of the panel, measured as the total thickness of the substrate and interlayer film, is at least about 2 mm, at least about 3 mm, at least about 3.5 mm, at least about 4 mm, at least about 4.5 mm, at least about 4.65 mm. At least about 4.75 mm, or at least about 5 mm, and / or about 6.5 mm or less, about 6.25 mm or less, about 6.0 mm or less, about 5.75 mm or less, about 5.5 mm or less, or about 5 mm or less. It's okay. The thickness of one or both substrates can be substantially smaller than expected for conventional multilayer panels. For example, in some embodiments, the total thickness of each of the hard substrates is about 4.0 mm or less, about 3.9 mm or less, about 3.8 mm or less, about 3.7 mm or less, about 3.6 mm or less, about. It can be 3.5 mm or less and about 3.4 mm or less.

A multilayer panel can be formed using any suitable hard substrate, and in some embodiments, the substrate may be glass, polycarbonate, biaxially oriented PET, copolyester, acrylic resin, and the like. A material selected from the group consisting of these combinations can be included. If the hard substrate contains a polymer material, the polymer material may or may not include a hard coat surface layer. In some embodiments, the rigid substrate may have a refractive index lower than that of the interlayer film used to form the multilayer panel. For example, the refractive index of at least one of the hard substrates is about 1.550 or less, about 1.545 or less, about 1.540 or less, about 1.535 or less, about 1.530 as measured as described above. It may be less than or equal to, or about 1.525 or less. In some embodiments, the index of refraction of at least one of the rigid substrates is at least about 5%, at least about 10%, at least about 15%, at least about about the index of refraction of the interlayer film used to form the multilayer panel. It may be 20% lower. In some embodiments, the index of refraction of one or both substrates is at least about 0.25 units, at least about 0.50 units, at least about 0.75 units, and at least about 1. It may be 0 units, at least about 1.1 units, or at least about 1.5 units lower. Alternatively, it can be said that the refractive index of the interlayer film is higher than that of at least one of the substrates by the amount or percentage described here.

[0134] A multilayer panel constructed according to some aspects of the present invention can have an equivalent index of refraction higher than one or more refractive indexes of a rigid substrate. The term "equivalent index of refraction" as used herein refers to the overall index of refraction of a composite material, such as a multilayer panel. The equivalent index of refraction ( _neq ) of a particular multilayer panel is calculated according to the following equations (1) and (2).

In the formula, x _T and t _T are defined as follows.

In the above equation, θ _eq is the equivalent angle of incidence _{of the complex, x T} is the distance that light travels through the entire complex, and t _T is the total thickness of the complex with m layers. in and, n _a is the refractive index of air, theta ₁ is the incident angle of the light passing through the air interface / layer 1, n _eq is the equivalent refractive index of the composite, t _i is the layer _i It is the thickness, and θ _i is the incident angle of light passing through the _{layer i.} The equivalent index of refraction of the multilayer panels described herein is at least about 1.490, at least about 1.495, at least about 1.500, at least about 1.505, at least about 1.510, at least about 1.515. It can be at least about 1.520, at least about 1.525, at least about 1.530, at least about 1.535, at least about 1.540, or at least about 1.545.

[0136] In some embodiments, the multilayer panel is at least about 0.25%, at least about 0.5%, and at least about 0% of the index of refraction of at least one of the substrates used to form the multilayer interlayer film. It can have an equivalent index of refraction that is .75%, at least about 1%, or at least about 1.5% higher. For example, the panel has an equivalent index of refraction that is at least 0.010, at least about 0.015, at least about 0.020, or at least about 0.025 higher than the index of refraction of one or more hard substrates used to form the panel. Can have. In some embodiments, the equivalent index of refraction of the multilayer panel can be lower than the index of refraction of the interlayer film used to form the panel, eg, the index of refraction of the interlayer film used to form the multilayer panel. At least about 0.5%, at least about 1%, at least about 1.5%, at least about 2%, at least about 2.5%, at least about 3%, at least about 5%, or at least about 7% lower than be able to. The difference between the refractive index of the interlayer and the equivalent index of refraction of the panel is at least about 0.010, at least about 0.025, at least about 0.050, at least about 0.10, at least about 0.125, at least about 0. It can be .50, or at least about 0.75.

[0137] The multilayer panels described herein include, for example, panels, windows, doors for various transportation applications such as automobile windshields and windows, aircraft windshields and windows, marine applications, railroad applications, and the like. Used for a variety of end applications such as structural building panels such as stairs, passages, ballasts, decorative building panels, weatherproof panels such as hurricane glass or tornado glass, bulletproof panels, and other similar applications. be able to.

[0138] In some embodiments, the multilayer panels described herein are double or reflective that interfere with each other when used, for example, to project a heads-up display (HUD) image onto the windshield of an automobile or aircraft. A reduction in "ghost" images can be shown. Ghost images are usually most problematic when the windshield has a generally uniform thickness profile due to the difference in its position as the projected image reflects off the inner and outer surfaces of the glass. However, in some embodiments, the multilayer panels described herein minimize the projection of ghost images so that, for example, the panels have a much shorter double image separation distance than those indicated by conventional panels. Can be.

[0139] A method of measuring double image separation comprises providing a multilayer panel containing at least a pair of hard substrates and interlayers arranged between them. The interlayer film can include any property of any interlayer film described herein, or the interlayer film may be any interlayer film described herein. In some embodiments, the interlayer film may be a tapered interlayer film that includes, for example, at least one tapered area having a wedge angle of at least 0.05 mrad. The substrate can also include one or more of the properties of the substrates described herein, and in some embodiments, the substrate can include glass.

[0140] To measure the double image separation of a given panel, a projected image can be generated by passing light through at least a portion of the panel. In some embodiments, the light passing through the panel comprises an image such as a grid, line, shape, or image. In some embodiments, the image can be generated by reflecting the display of the thin film transistor onto a substantially flat, mirror-finished surface, but other suitable methods of producing the image can be used. .. When the multilayer panel is formed by using the tapered interlayer film, at least a part of the light passing through the panel can pass through at least a part of the tapered area. Alternatively, or even more, the light may pass through one or more other target areas along the panel to measure the double image separation formed as the light is projected through these areas. Can be.

[0141] Once the light has passed through the surface of the panel and is reflected off the surface, a projected image can be projected onto the surface and then imaged to form a captured image. In some embodiments, the projected image displayed on the surface may include a primary image and a secondary "ghost" image that is slightly overlapped from the primary image, as shown in FIG. .. The projected image can be imaged using a digital camera or other suitable device, and the imaging can include digitizing the projected image to form a digital projected image containing a plurality of pixels.

[0142] Once digitized, the captured image can be quantitatively analyzed to form a profile that includes at least one primary image index and at least one secondary image index. The analysis can be performed by converting at least a portion of the digital projection image into a vertical image matrix containing numerical values representing the intensity of the pixels in that portion of the image. Next, as shown in FIG. 11, the columns of the matrix can be extracted and graphed for the number of pixels to give a profile. Next, the difference can be obtained by comparing the primary image index of the profile with the secondary image index of the profile. In some embodiments, the primary image index can include the highest intensity peak of the graph, while the double image index can include the lower intensity peak. Any suitable difference between the two indicators can be determined, and in some embodiments this may be the difference in position between the two indicators in the profile graph. Based on this difference, the double image separation distance for the part of the panel tested can be calculated. Specific use of the above method for determining the double image separation distance is described in Example 11.

[0143] Multilayer panels constructed according to a plurality of aspects of the present invention can have a much lower duplex image separation distance than panels formed by conventional methods. For example, in some embodiments, the double image separation distance of the panels described herein has a refractive index of, for example, less than 1.480, and all other matters are equivalent. It can be at least about 10%, at least about 20%, at least about 30%, and at least about 40% shorter than the double image separation distance of the panel formed from. The double image separation distance for a given panel may be determined, in part, by its specific configuration, such as the type and dimensions of its interlayer film and substrate. Specific examples of double image separation distances for some panels of the present invention and comparative panels are given in the examples.

[0144] When laminating a polymer layer or interlayer between two hard substrates such as glass, the process involves at least the following: (1) assembling the two substrates and interlayer; (2). The assembly is heated for a first short time by an IR radiator or convection device; (3) the assembly is passed through a pressurized nip roll for the first degassing; (4) the assembly is passed at about 60 ° C to about 120 ° C. Heat briefly to give the assembly sufficient temporary adhesion to seal the edges of the interlayer; (5) pass the assembly through a second pressure nip roll to pass the edges of the interlayer. Further sealing allows for further handling; and (6) the assembly is autoclaved at a temperature between 135 ° C. and 150 ° C. and a pressure between 150 psig and 200 psig for about 30-90 minutes; including steps. be able to. Other methods for degassing the interlayer-glass interface described in steps (2)-(5) above according to some embodiments include vacuum bag and vacuum ring processes, both of which It can be used to form the interlayer film of the present invention described herein.

[0145] In some embodiments, the multilayer panel may include at least one polymer film arranged on a layer or interlayer film to form a multilayer panel called a "double layer". In some embodiments, the interlayer film used in the bilayer can include a multilayer interlayer film, while in other embodiments, a monolith type interlayer film can be used. The use of polymer films in the multilayer panels described herein can improve the optical properties of the final panel while also providing other performance improvements such as infrared absorption. Polymer films differ from polymer layers or interlayers in that the film alone does not provide the required penetration resistance and glass retention properties. The polymer film may also be thinner than the sheet and may have a thickness in the range of 0.001-0.25 mm. Poly (ethylene terephthalate) (PET) is an example of a material used to form a polymer film.

[0146] The following examples are intended to illustrate the invention in order to teach those skilled in the art to manufacture and use the invention, and are not intended to limit the scope of the invention in any way.
[0147] The following examples describe the production of several resin compositions, layers, and interlayers, including various poly (vinyl acetal) resins. The sound insulation and optical properties of various comparative materials and materials of the invention were evaluated using several tests performed on many compositions, layers, and interlayer films, as described below.

Example 1: Production of high refractive index poly (vinyl acetal) resin:
[0148] One or more aldehydes, including n-butyraldehyde (nBuCHO; RI = 1.377), isobutyraldehyde (iBuCHO; RI = 1.374), and 2-ethylhexyl aldehyde (2EHCHO; RI = 1.414). By acetalizing polyvinyl alcohol using the above, several comparative poly (vinyl acetal) resins called comparative resins CR-1 to CR-12 in Table 2 below were prepared. The composition of the obtained resin was measured using either the ASTM-D1396 or the FT-IR / SEC method described in detail above. In addition, the refractive index and glass transition temperature (T _g ) of some resins are also measured according to the method described above, and the results are given in Table 2 below.

[0149] Further, several poly (vinyl acetal) resins according to a plurality of aspects of the present invention were also prepared in a similar manner. These resins of the present invention (referred to as the resins of the present invention DR-1 to DR-21 in Table 3) include n-butyraldehyde, benzaldehyde (BzCHO; RI = 1.545), and cinnamaldehyde (CCHO; RI = 1. 620), various including 4-chlorobenzaldehyde (4-ClBzCHO; RI = 1.5850), 2-phenylpropionaldehyde (2PHPrCHO; RI = 1.517), and hydrocinnamaldehyde (HCCHO; RI = 1.523). It was formed by acetalizing polyvinyl alcohol with a mixture of high refractive aldehydes. The refractive indexes of some of the resins of the present invention were also determined, and the results are summarized in Table 3 below.

[0150] As shown in Tables 2 and 3 above, polyvinyl acetal resins containing residues of at least one high refractive aldehyde, including those shown above, are n-butyraldehyde, isobutyraldehyde, and 2-. It tends to exhibit higher refractive index than those containing aldehyde residues such as ethylhexyl aldehyde.

Example 2: Production of high refractive index resin interlayer film:
[0151] Some of the comparative resins shown in Table 2 above and some of the resins of the present invention shown in Table 3 were combined with various amounts of the plasticizer triethylene glycol bis (2-ethylhexanoate) (3GEH). By mixing and melt blending, some comparisons and interlayer films of the present invention were formed. The composition, refractive index, and glass transition temperature of each of the obtained interlayer films (referred to as comparative interlayer films CL-1 to CL-14 and the intermediate films DL-1 to DL-26 of the present invention) are as described above. The measurements are taken and the results are summarized in Tables 4 and 5, respectively.

[0152] As shown in Tables 4 and 5, the interlayer film of the present invention using the resin of the present invention having a higher refractive index from Table 3 is a resin having a lower refractive index such as the comparative resin shown in Table 2. It shows a higher refractive index than the comparative interlayer film prepared using. Furthermore, as shown by comparing the interlayer films DL-1 and DL-2 and DL-6 and DL-23 to DL-25 of the present invention, the amount of plasticizer used to form the interlayer film is a layer. It affects both the glass transition temperature and the refractive index of the resin, but not necessarily the same for all resins. For example, as shown by comparing DL-1 (75 phr 3GEH; DR-1) and DL-2 (50 phr 3GEH; DR-1), reducing the amount of plasticizer by about 33% reduces the interlayer film. The glass transition temperature of the glass increases by 11 ° C. (from 1 ° C. to 12 ° C.), but the refractive index increases by only 0.006 (from 1.473 to 1.479). However, as shown by comparing DL-25 (60 phr 3GEH; DR-5) and DL-6 (75 phr 3GEH; DR-5), the plasticizer content in the layer formed by this resin When reduced, the glass transition temperature rises only 1 ° C. (from 1 ° C. to 2 ° C.), while the index of refraction increases by 0.004 (from 1.484 to 1.488).

Example 3: Production of an interlayer film using a high refractive index resin:
[0153] Several comparative and multilayer interlayer films of the present invention, which were formed in Example 2 and summarized in Tables 4 and 5 above, respectively, were used to generate several comparative and multilayer interlayer films of the present invention. Each multilayer interlayer sandwiches an inner "core" layer with a thickness of 5 mils, usually formed of a resin with a lower residual hydroxyl content, a pair with a total thickness of 28 mils. Included an outer "skin" layer of. The composition of the interlayer film and some properties including refractive index, glass transition temperature, color spots, and loss factor were measured as described above, and the comparative multilayer interlayer film (CI-1 to CI-16) and the present. The results regarding the multi-layer interlayer film (DI-1 to DI-29) of the present invention are summarized in Tables 6 and 7 below.

[0154] As shown in Table 6 above, interlayer films formed from skin and core layers with a refractive index difference of 0.010 or greater show optical defects as indicated by color spot values higher than 5. rice field. However, as shown in Table 7, the interlayer film formed from the skin and core layers having a difference in refractive index of less than 0.010 showed a low color spot value of 1 or less. Moreover, as shown in Table 7, such low color spot values are higher or lower refraction than the skin layer, as long as the absolute value of the difference between the indices of refraction of adjacent layers is less than 0.010. It could be achieved by an interlayer film with a core layer having a rate. Also, as shown in Table 7, interlayer films formed from skin and core layers with both high RI aldehyde residues and refractive index differences greater than 0.010 have high color spot values of 5 or greater. Indicated.

Example 4: Stability of multilayer interlayer film:
[0155] Two comparative multilayer interlayer films manufactured as described in Examples 1 to 3 above, CI-2 and CI-7, and two multilayer interlayer films of the present invention, DI-4 and DI-5, were tested. Then, the relative stability of the interlayer film with the passage of time was determined. Net plasticizer transfer was measured by comparing the glass transition temperature of each layer at the first time point (t = 0) and after the layers reached equilibrium. The results are summarized in Table 8 below.

[0156] The interlayer film DI-4 of the present invention (as well as the comparative interlayer films CI-2 and CI-7) showed the smallest change in the glass transition temperature of both the skin and core layers of the interlayer film in equilibrium. This indicates a small amount of plasticizer transfer between the skin and core layers of the interlayers CI-2, CI-7, and DI-4, respectively. Comparative interlayers CI-2 and CI-7 may be relatively stable, but both show color spot values greater than 5, which is unacceptable for most optical applications. In contrast, the color spot value indicated by the interlayer film DI-4 of the present invention was less than 1.

[0157] The slight decrease in glass transition temperature exhibited by the interlayer film DI-5 of the present invention in equilibrium indicated that a small amount of plasticizer was transferred from the skin layer to the core layer. Such movement can be mitigated by using a smaller amount of plasticizer in the skin layer or a larger amount in the core. Nevertheless, the refractive indexes of the core layer and the skin layer of the interlayer film DI-5 of the present invention differed by only 0.004, and as a result, this interlayer film also showed a color spot value of less than 1.

Example 5: Blended poly (vinyl acetal) resin:
[0158] Some comparative resins and resins of the invention prepared as described in Example 1 above were mixed and melt blended with 38 phr of 3GEH plasticizer to make comparative blended layers CBL-16 and CBL. -17, as well as the blended layers DBL-27 and DBL-28 of the present invention were formed. The comparative polymer layer CL-2 is shown in Table 4. The comparative polymer layer CL-15 was prepared using 3GEH of the comparative resins CR-10 and 38 phr, while the polymer layers DL-27 and DL-28 of the present invention were prepared using the resins DR-3 and DR-5 of the present invention, respectively. Also prepared using 38 phr of 3GEH. Cloudiness and visible transmittance (%) ( _Tvis ) for each blended resin interlayer were measured along with cloudiness and visible transmittance (%). The results are given in Table 9 below.

[0159] As shown in Table 9 above, the comparative blended interlayer films CBL-16 and CBL-17 formed from the blend of the comparative resins CR-2 and CR-10 have high color spot values and comparative resins. It showed a lower visible transmittance (%) than the single polymer layer of CR-2 (comparative layer CL-2) or the single polymer layer of CR-10 (comparative interlayer film CL-15). On the other hand, the present invention formed from a blend of the comparative resin CR-2 and the resin of the present invention having a high refractive index (resin DR-3 in the layer DBL-27 or resin DR-5 in the layer DBL-28). The blended interlayer films DBL-27 and DBL-28 showed substantially the same degree of cloudiness and visible transmittance (%) as the comparative interlayer film CL-2 prepared using only the comparative resin CR-2. Therefore, even if the high refractive index resin of the present invention is added to the comparative interlayer film, the optical quality of the obtained interlayer film is not deteriorated.

Example 6: Production of an interlayer film having a high refractive index additive:
[0160] Several poly (vinyl acetal) resins were prepared by acetalizing polyvinyl alcohol with n-butyraldehyde. Resins with different residual hydroxyl contents were melt-blended with different amounts of 3GEH plasticizers and used to form different layers of multilayer interlayers. Each interlayer had an inner "core" layer with a thickness of 5 mils sandwiched between two outer "skin" layers, each having a thickness of 14 mils. The poly (vinyl butyral) resin used to form the core layer had a hydroxyl content of 11% by weight, and the resin used for the skin layer had a hydroxyl content of 19% by weight. Both resins had a residual acetate content of about 2% by weight.

[0161] Using a polymer layer plasticized with 3GEH, it was present in various amounts in the core and skin layers to form comparative interlayer films CI-17 to CI-19. In addition to 3GEH, the interlayer film DI-30 to DI-38 of the present invention contains various amounts of two different high refractive index additives: Bensoflex® 2-45 (diethylene glycol dibenzoate; Eastman Chemical Company). (Commercially available from Kingsport, Tennessee) (Additive A-1) (has a melting point of 28 ° C. and a refractive index of 1.542); and Bensoflex® 352 (1,4-cyclohexane) Dimethanol dibenzoate; commercially available from Eastman Chemical Company) (additive A-2) (having a melting point of 118 ° C. and a refractive index of 1.554); was also included. The refractive index and the glass transition temperature of each of the comparative interlayer films CI-17 to CI-19 and the interlayer films DI-30 to DI-38 of the present invention were measured, and the results are summarized in Table 10 below.

[0162] As shown in Table 10 above, increasing the plasticizer content of the core layer of the interlayer film containing only the 3GEH plasticizer lowers the glass transition temperature of the layer, and finally its sound insulation performance. Has improved. However, such an increase also widened the difference between the indices of refraction of the skin layer and the core layer, thereby degrading the optical quality of the interlayer film. As shown by comparing the interlayer films DI-30 to DI-38 of the present invention in Table 10, the refractive index of the core layer prepared by using the higher refractive index additive increases the plasticizer loading amount. It remained almost constant with it, while still showing a similar decrease in glass transition temperature. As a result, an interlayer film having a core and a skin layer having substantially the same refractive index was obtained, which greatly reduced optical defects such as color spots. At the same time, the core layer also showed a sufficiently low glass transition temperature, indicating that the resin also had sound insulation properties.

Example 7: Production of a core layer having a reactive high refractive index additive:
[0163] The inner core layer of the multilayer interlayer is formed by melt-blending a polyvinyl n-butyral resin having a residual hydroxyl content of 11% by weight and a residual acetate content of about 2% by weight with various amounts of 3GEH plasticizer. Several polymer layers were formed for use in the simulation. The comparative layer CL-16 contains 75 phr of 3GEH, while the layers DL-29 to DL-31 of the present invention contain various mixtures of 3GEH and a reactive high refractive index additive (highly reactive RI additive). Prepared using. The reactive high RI additive (Additive A) used in layers DL-29 and DL-30 of the present invention is diphenyldimethoxysilane (commercially available as SID4535.0 from Gelest Inc., Morrisville, Pennsylvania). The reactive high RI additive (Additive B) used in layer DL-31 of the present invention was phthalic anhydride (commercially available from Sigma Aldrich Co., St. Louis, Missouri). The refractive indexes of the comparative layers CL-16 and the layers DL-29 to DL-31 of the present invention were measured, and the results are shown in Table 11 below.

[0164] As shown in Table 11, a polymer layer formed by using 3GEH in combination with one or more reactive high index additives has a higher index of refraction than a polymer layer prepared using only 3GEH. Had had. As a result, when used as the inner core layer in the multilayer interlayer film, the layers DL-29 to DL-31 of the present invention are dense due to the refractive index (RI = 1.477) of the skin layer formed of polyvinyl n-butyral. It had a refractive index matching that of. As a result, the multilayer interlayer film formed by using the layers DL-29 to DL-31 of the present invention as the core layer has fewer optical defects than the multilayer interlayer film formed by using the comparative layer CL-16 as the inner core layer. show.

Example 8: Various interlayer films using a resin blend having a high refractive index plasticizer:
[0165] Two types of polyvinyl n-butyral resins R-1 and R-2 were prepared according to the procedure described above in Example 1. Resin R-1 had a residual hydroxyl content of 19% by weight, while resin R-2 had a residual hydroxyl content of 11% by weight. Both resins had a residual acetate content of 2% by weight. Several resin blends were prepared containing different amounts of resins R-1 and R-2 to simulate different blend ratios. This blend was formulated with 3GEH (Plasticizer P-1; RI = 1.442), Dioctyl Phthalate (Plasticizer P-2; RI = 1.485), 30% by weight 3GEH and 70% by weight Bensoflex®. A blend of 2088 (commercially available from Eastman Chemical Company, Kingsport, Tennessee) (plasticizer P-3; RI = 1.506), and nonylphenyltetraethylene glycol (plasticizer P-4; RI = 1.500). ) Was mixed with a 38 phr plasticizer selected from. Next, the obtained plasticized resin containing both resins and a plasticizer was molded into a single sheet. The refractive index, cloudiness, and visible transmittance (%) for each sheet are obtained, and the results are given in Table 12 below.

[0166] As shown in Table 12 above, the blended polymer layers prepared with the plasticizer P-1 are substantially as the amount of R-2 in the resin with the lower hydroxyl content increases. The optical properties of these resin blends, which maintained a constant index of refraction but had high levels of R-2, deteriorated as the amount of R-2 increased. For example, as shown in Table 12, the cloudiness of blends containing more than 1.1% resin R-2 increased, while the visible transmission (%) of these blends was 88.5% to 81. It decreased to 0.7%.

[0167] On the other hand, each resin blend containing more than 2.2% of the resin R-2 plasticized with the higher refractive index plasticizers P-2 to P-4 has a smaller amount of the resin R. It showed substantially the same degree of cloudiness and visible transmittance (%) as the blend having -2. Therefore, resin blends with higher refractive index plasticizers such as the plasticizers P-2 to P-4 will contain more resin with a lower hydroxyl content without adversely affecting the optical properties of the final blend. It can be concluded that it can be made possible to use in.

Example 9: Poly (vinyl butyral) layer containing a high refractive index plasticizer:
[0168] Several poly (vinyl n-butyral) resins (PVB-1 to PVB-3) are mixed and melt-blended with different types and amounts of plasticizers. ) A layer was formed. Each of the resins PVB-1 to PVB-3 has a different residual hydroxyl content in the range of 11 to 20.4% by weight, and all three resins have a residual vinyl acetate content of 1% by weight. rice field. Comparative layers CL-17 to CL-19 were prepared using various amounts of triethylene glycol di (2-ethylhexanoate) (3GEH; RI = 1.442), while layers DL-32 to the present invention. DL-37 contained a mixture of 3GEH and Bensoflex® 354 (commercially available from Eastman Chemical Company, Kingsport, Tennessee) (RI = 1.53). The refractive index of each layer is measured, and the results are summarized in Table 13 below.

[0169] As shown in Table 13 above, the polymer layer containing the high refractive index plasticizer exhibited a higher refractive index than that containing only the low refractive index plasticizer.
Example 10: Production of an interlayer film having a high refractive index additive:
[0170] Using some of the comparisons and interlayer films of the present invention formed in Example 9 and summarized in Table 13 above, some comparisons and multilayer interlayer films of the present invention were produced. Each multilayer interlayer sandwiches an inner "core" layer with a thickness of 5 mils formed of a resin with a lower residual hydroxyl content, and a pair of outer "cores" with a thickness of 14 mils each. Included a "skin" layer. As described above, the composition of the multilayer interlayer film and some properties such as total plasticizer content, refractive index, glass transition temperature, color spot, and loss coefficient were measured, and the comparative multilayer interlayer film CI-20 and CI were measured. Table 14 below summarizes the results of -21 and the multilayer interlayer films DI-39 to DI-41 of the present invention.

[0171] As shown in Table 14 above, the interlayer film formed from the skin and core layers having a difference in refractive index greater than 0.010 shows more optical defects as indicated by the color spot value of 5. rice field. Furthermore, the interlayer films DI-39 to DI-41 of the present invention using a high refractive index plasticizer are compared with the comparative interlayer films CI-20 and CI-21 using only a plasticizer having a refractive index of less than 1.460. Showed a higher overall index of refraction.

Example 11: Comparison with various thicknesses and wedge angles and measurement of double image separation distance for the multilayer panel of the present invention:
[0172] A mixture obtained by mixing a poly (vinyl butyral) resin having a residual hydroxyl content of 18.7% by weight with a 38 phr plasticizer, triethylene glycol bis (2-ethylhexanoate) (3GEH). By extruding to form a single layer sheet, several interlayer films were formed. Several comparisons of forming an interlayer sheet with a uniform thickness of about 30 mils (about 0.76 mm) without flat or tapered areas and cutting it to have a wedge angle of 0 °. An interlayer film was formed.

[0173] Several sheets were formed, each with a tapered area, each with a different constant wedge angle, and each sheet was cut to form several tapered monolithic interlayers. The tapered interlayers each had a wedge angle in the range of 0.30 to 0.73 mrad. Each interlayer sample was then laminated between a pair of 6 "x 12" glass sheets (each glass / interlayer / glass multilayer panel was 3.0 mm, 4.32 mm, or 5. It had a thickness of 0 mm). The specific configurations of the comparative multilayer panels (CP-1 to CP-3) and the multilayer panels of the present invention (DP-1 to DP-15) are shown in Table 15 below.

[0174] Each of the laminates shown in Table 15 was subjected to a double image separation test using the apparatus 100 shown in FIG. As shown in FIG. 9, the test apparatus 100 includes a projector 130, an adjustable mirror 140, and a detector 120. The distance between the projector 130 shown as line A in FIG. 9 and the adjustable mirror 140 is 43.8 cm, and the distance between the adjustable mirror 140 shown as line B in FIG. 9 and the panel 110 is 31.7 cm. The distance between the panel 110 shown as line C in FIG. 9 and the detector 120 was 47 cm. _{Further, the incident angle at which the light from the projector 130 shown as θ 1} in FIG. 9 collides with the adjustable mirror 140 is 30.11 °, and the panel 110 is from the mirror 140 to the panel 110 shown as _{θ 2 in FIG.} the incident angle of the image of the above, and the light reflected from the panel 110 to the detector 120, shown as theta _{2 'are} respectively arranged to be equal to 24.8 ° in approximately equal. Finally, the panel 110 was aligned at an angle of 30.5 ° from the vertical line, as shown by _{θ 3} in FIG.

[0175] In order to measure the double image separation distance of the panel 110 using the apparatus 100 shown in FIG. 9, an image is generated using a standard thin film transistor display and reflected by the flat surface of the mirror 140 on the panel 110. I let you. The image was reflected onto one or more surfaces of the panel 110 and projected onto the detector 120. Next, an image is recorded using a digital camera to form an captured image as shown in FIG. 10, and then the digital image is an element (grayscale level) representing the intensity of each pixel of the digital image. The profile was formed by analysis by converting to a matrix having. Next, as shown in FIG. 11, the matrix was plotted as a function of the number of pixels for each column. The higher intensity peaks shown in FIG. 11 represented the primary image reflected from the panel, while the shorter, lower intensity peaks corresponded to the secondary or "ghost" images. Next, the separation distance (pixels) between the primary peak and the secondary peak is obtained, and using this, the following equation:

The double image separation distance (D) for each panel was calculated according to.
[0176] Using the procedure described above, the double image separation distances for each of the comparison panels (CP-1 to CP-3) and each of the panels of the present invention (DP-1 to DP-15) were measured. The results are given in Table 15 above. The results are also graphed in FIG.

[0177] In addition, some additional comparative multilayer panels (CP-4 to CP-8) and multilayer panels of the present invention (DP-16 to DP-29) are provided in a manner similar to that described above. However, it was constructed with varying thicknesses at several different wedge angles. Next, the double image separation test described above is performed on each of the comparative panels CP-4 to CP-8 and the panels DP-16 to DP-29 of the present invention, and the results are given in Table 16 below. FIG. 13 shows the double image separation distance as a function of the wedge angle with respect to the comparison panels CP-4 to CP-8 and the panels DP-16 to DP-29 of the present invention of various glass structures.

Example 12: Some comparisons and measurement of the equivalent index of refraction ( _neq ) for the multilayer panel of the present invention:
[0178] In the following examples, the equivalent refractive index: _neq of the comparative multilayer panel and the multilayer panel of the present invention was determined. PVB interlayers with a uniform thickness of 0.76 mm and a refractive index of 1.475 are laminated between glass panels, one with a thickness of 1.6 mm and the other with a thickness of 2.3 mm. By doing so, a comparison panel (CP-A) was formed. Each glass panel had a refractive index of 1.52 as measured at a wavelength of 589 nm and 25 ° C. according to ASTM-D542. When the equivalent refractive index of the comparison panel was obtained according to the above equations (1) to (4) at an incident angle of 60 ° (θ _{2), it was 1.512.}

[0179] Similarly, two glass panels having another PVB interlayer film having a uniform thickness of 0.76 mm, each having the same thickness as the panel used to form the comparative multilayer panel. The multilayer panel (DP-B) of the present invention was formed by laminating between the two. However, the PVB interlayer film used to form the multilayer panel (DP-B) of the present invention had a refractive index of 1.65. When the equivalent refractive index of the multilayer panel of the present invention was calculated using the above formula, it was 1.540. The DP-B of the multilayer panel of the present invention can show a practical maximum value (or a practical limit value) of the equivalent refractive index that can be achieved in some cases. The results are summarized in Table 17 below.

Example 13: Effect of index of refraction on double image separation for various laminates:
[0180] Several glass / air / glass laminates were formed to simulate multilayer panels with different equivalent indices of refraction. Each laminate was constructed by separating several glass sheets of varying thickness from each other using metal shims of appropriate dimensions to form and hold voids between the glass sheets. The total thickness of the obtained glass / air / glass laminate was maintained between 4 and 5 mm, and the equivalent refractive index for each was calculated according to the above formulas (1) to (4). The specific configurations of the two representative panels AGL-1 and AGL-2 and the values of the parameters of the above equations (1) to (4) are summarized in Tables 18 and 19, respectively.

[0181] Next, each of the glass / air / glass panels formed as described above is subjected to a double image separation test similar to that described in Example 11 above using the apparatus shown in FIG. I went to the glass. However, the captured images formed during the analysis of these panels contained three double images instead of one due to the large difference between the refractive indexes of glass and air. For this analysis, the separation between the primary image and the last double image was analyzed when determining the double image separation distance for each panel. The results of these analyzes are summarized in a graph in FIG.

[0182] The invention has been disclosed in connection with the description of some embodiments, including those currently considered to be preferred embodiments, but the detailed description is for illustrative purposes only and is understood to limit the scope of the invention. should not do. As will be appreciated by those skilled in the art, aspects other than those described in detail herein are included in the present invention. Modifications and modifications of the described embodiments may be made without departing from the spirit and scope of the invention.

[0183] Further, any range, value, or feature given with respect to any single component of the invention is given with respect to any other component of the invention, where compatible. It is understood that it can be used interchangeably with any range, value, or feature provided to form an embodiment having the values specified for each component given throughout the specification. For example, in addition to containing any range of plasticizers given, an interlayer film containing poly (vinyl butyral) having a given range of residual hydroxyl content is formed to form the scope of the invention. Although inside, many variants can be formed that are cumbersome to list. Furthermore, the scope given for a genus or category such as phthalate or benzoate can also be applied to species within the genus or component of that category, such as dioctyl terephthalate, unless otherwise indicated. ..
The present invention includes the following embodiments.
[1] Containing at least one polymer layer containing a poly (vinyl acetal) resin and at least one plasticizer, the polymer layer has a refractive index of at least 1.480, and the interlayer film is 0.85 mrad or less overall. A tapered interlayer containing a tapered area with a wedge angle.
[2] The interlayer film according to [1], wherein the tapered area has an overall rust angle of less than 0.55 mrad, and the polymer layer has a refractive index of at least 1.500.
[3] The interlayer film according to [1], wherein the interlayer film is a monolith type intermediate film.
[4] The interlayer film is a multilayer interlayer film containing a polymer layer and another polymer layer adjacent to the polymer layer, and the difference between the glass transition temperature of the polymer layer and the glass transition temperature of the other polymer layer is at least. The interlayer film according to [1], which has a temperature of 3 ° C.
[5] The other polymer layer contains a second poly (vinyl acetal) resin and at least one plasticizer, and the residual hydroxyl content of the poly (vinyl acetal) resin in the polymer layer and the second in the other polymer layer. The interlayer film according to [4], wherein the difference between the residual hydroxyl contents of the poly (vinyl acetal) resin is at least 2% by weight.
[6] The interlayer film according to [1], wherein the tapered area includes an area of at least one variable angle having a curved thickness profile and a continuously changing wedge angle.
[7] The interlayer film according to [1], wherein the tapered area includes at least one constant angle area having a linear thickness profile and a constant wedge angle.
[8] Containing a pair of hard substrates and the interlayer film according to [1], the interlayer films are arranged between a pair of hard substrates, and the hard substrates have a total thickness of less than 4.0 mm. Multi-layer panel with.
[9] A pair of hard substrates; and
An interlayer film that is located between the substrates and contains a tapered area with an overall rust angle of less than 0.85 mrad;
Including;
A multilayer panel in which the equivalent index of refraction of the multilayer panel is at least 0.010 higher than that of each of the rigid substrates.
[10] The panel according to [9], wherein the multi-layer panel has an equivalent refractive index of at least 1.500.
[11] The panel according to [9], wherein the refractive index of each of the substrates is at least 20% lower than the refractive index of the interlayer film.
[12] The panel according to [9], wherein the refractive index of the interlayer film is at least about 1.600.
[13] The panel according to [9], wherein the tapered area has an overall rust angle of less than 0.55 mrad.
[14] The interlayer film contains at least one polymer layer containing a poly (vinyl acetal) resin and at least one plasticizer, and the total thickness of each of the hard substrates is 4.0 mm or less, according to [9]. Described panel.
[15] The interlayer film comprises a multilayer interlayer film each containing a poly (vinyl acetal) resin and two or more polymer layers containing at least one plasticizer, and the interlayer film has at least two glass transition temperatures. The panel according to [14], wherein the difference between the two glass transition temperatures is at least about 3 ° C.
[16] A pair of hard substrates; and
Tapered interlayer film located between the substrates and containing at least one polymer resin;
Including;
A multilayer panel in which the refractive index of the interlayer film is at least 5% higher than the refractive index of each of the hard substrates.
[17] The tapered portion comprises a tapered region having a wedge angle of 0.85 mrad or less, and the interlayer film comprises at least one polymer layer having a refractive index of at least about 1.480, according to [16]. panel.
[18] The panel according to [16], wherein the panel has an equivalent refractive index higher than the respective refractive index of the hard substrate.
[19] The interlayer film is a multilayer interlayer film containing at least a first polymer layer and a second polymer layer adjacent to the first polymer layer, and the first polymer layer is a first poly (vinyl acetal) resin. And at least one plastic agent, the second polymer layer contains a second poly (vinyl acetal) resin and at least one plastic agent, the glass transition temperature of the first polymer layer and the second polymer layer. The difference between the glass transition temperatures of the first poly (vinyl acetal) resin is at least 3 ° C, and the difference between the residual hydroxyl content of the first poly (vinyl acetal) resin and the residual hydroxyl content of the second poly (vinyl acetal) resin is at least 2 weights. %, The panel according to [16].
[20] The interlayer film has a minimum thickness in the range of about 0.25 to about 1.2 mm and a maximum thickness in the range of about 0.38 to about 2.2 mm, and has a minimum thickness of the interlayer film and a minimum thickness of the interlayer film. The panel according to [16], wherein the difference between the maximum thicknesses is at least about 0.13 mm and the total thickness of each of the hard substrates is less than about 4.0 mm.

Claims (14)

Comprises a poly (vinyl acetal) at least one polymeric layer comprising a resin and at least one plasticizer, the polymer layer has a refractive index of at least 1.480, the entire intermediate layer is 0.50 to 0.85 mrad A tapered interlayer containing a tapered area with a target wedge angle. Po Rimmer layer has a refractive index of at least 1.500, an intermediate film according to claim 1. The interlayer film according to claim 1 or 2, wherein the interlayer film is a monolith type intermediate film. The interlayer film is a multilayer interlayer film containing a polymer layer and other polymer layers adjacent to the polymer layer, and the difference between the glass transition temperature of the polymer layer and the glass transition temperature of the other polymer layer is at least 3 ° C. The interlayer film according to claim 1 or 2. The other polymer layer contains a second poly (vinyl acetal) resin and at least one plasticizer, the residual hydroxyl content of the poly (vinyl acetal) resin in the polymer layer and the second poly (vinyl acetal) in the other polymer layer. The interlayer film according to claim 4, wherein the difference between the residual hydroxyl contents of the vinyl acetal) resin is at least 2% by weight. The interlayer film according to any one of claims 1 to 5, wherein the tapered area includes an area of at least one variable angle having a curved thickness profile and a continuously changing wedge angle. The interlayer film according to any one of claims 1 to 6, wherein the tapered area includes at least one constant angle area having a linear thickness profile and a constant wedge angle. A pair of hard substrates and an interlayer film according to any one of claims 1 to 7 are included, the interlayer films are arranged between a pair of hard substrates, and the hard substrates are a total of less than 4.0 mm. Multi-layer panel with thickness. A pair of hard substrates; and an interlayer film according to any one of claims 1 to 7 arranged between the substrates;
Including;
A multilayer panel in which the equivalent index of refraction of the multilayer panel is at least 0.010 higher than that of each of the rigid substrates. The panel according to claim 9, wherein the refractive index of each of the substrates is at least 20% lower than that of the interlayer film. The panel according to claim 9, wherein the refractive index of the interlayer film is at least about 1.600. A pair of hard substrates; and a tapered interlayer film according to any one of claims 1 to 7 arranged between the substrates;
Including;
A multilayer panel in which the refractive index of the interlayer film is at least 5% higher than the refractive index of each of the hard substrates. The panel according to claim 12, wherein the panel has an equivalent refractive index higher than each refractive index of the hard substrate. The interlayer film has a minimum thickness in the range of about 0.25 to about 1.2 mm and a maximum thickness in the range of about 0.38 to about 2.2 mm, and the minimum thickness of the interlayer film and the maximum thickness of the interlayer film. 12. The panel of claim 12, wherein the difference between the two is at least about 0.13 mm and the total thickness of each of the hard substrates is less than about 4.0 mm.

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