JP7559754B2 - Composition, flat plate-like molded body, and method for producing flat plate-like molded body - Google Patents

Description

The present invention relates to a composition, a flat-plate-shaped molded body, and a method for producing a flat-plate-shaped molded body.

Polycarbonate resins are used as molding materials for a variety of products. In particular, blending polycarbonate resins with other resins has been studied in order to impart various functions to the polycarbonate resins.
For example, Patent Document 1 discloses an in-vehicle air freshener container part formed from a resin composition obtained by blending 0.01 to 0.3 parts by mass of (C) a phosphate compound with 100 parts by mass of a polymer component consisting of (A) 20 to 60 parts by mass of a polyarylate resin and/or polycarbonate resin, and (B) 80 to 40 parts by mass of a polyester in which terephthalic acid is the main dicarboxylic acid component and 1,4-cyclohexanedimethanol accounts for 70 mol % or more of the diol component.
Moreover, Patent Document 2 describes blending a polyarylate resin having a specific structure with a polycarbonate resin.

JP 2004-002609 A JP 2013-076042 A

As mentioned above, blending various thermoplastic resins with polycarbonate resins has been investigated.
Here, the inventors have conducted research and found that when a polyarylate resin is blended with a polycarbonate resin and molded, transparency may be deteriorated.
The present invention has an object to solve the above problems, and has an object to provide a composition having excellent transparency, a flat plate-like molded product, and a method for producing the flat plate-like molded product.

（式（Ｂ－２）中、Ｒ^８は、それぞれ独立に、フッ素原子、塩素原子、臭素原子、ヨウ素原子、炭素原子数１～９のアルキル基、炭素原子数６～１２のアリール基、炭素原子数１～５のアルコキシ基、炭素原子数２～５のアルケニル基または炭素原子数７～１７のアラルキル基を表す。ｑは０～５の整数を表す。）
＜７＞前記組成物の示差走査熱量計で測定したガラス転移温度が１５０℃以上である、＜１＞～＜６＞のいずれか１つに記載の組成物。
＜８＞前記組成物を厚み５００μｍに成形した際のヘイズが５．０％以下である、＜１＞～＜７＞のいずれか１つに記載の組成物。
＜９＞さらに、酸化防止剤（Ｃ）を含む、＜１＞～＜８＞のいずれか１つに記載の組成物。
＜１０＞前記酸化防止剤（Ｃ）が、リン系酸化防止剤を含む、＜９＞に記載の組成物。
＜１１＞さらに、エステル交換防止剤（Ｄ）を含む、＜１＞～＜１０＞のいずれか１つに記載の組成物。
＜１２＞＜１＞～＜１１＞のいずれか１つに記載の組成物から形成された平板状成形体。
＜１３＞押出成形品である、＜１２＞に記載の平板状成形体。
＜１４＞厚みが１０～２０００μｍである、＜１２＞または＜１３＞に記載の平板状成形体。
＜１５＞＜１＞～＜１１＞のいずれか１つに記載の組成物を溶融押出することを含む、平板状成形体の製造方法。 As a result of investigations conducted by the present inventors in light of the above-mentioned problems, it was found that the above-mentioned problems could be solved by using a polycarbonate resin (A) having a small intrinsic viscosity and a polyarylate resin (B) having an intrinsic viscosity within a specified range, and by reducing the difference in intrinsic viscosity between the polycarbonate resin (A) and the polyarylate resin (B). Specifically, the above-mentioned problems were solved by the following means.
<1> A composition comprising a polycarbonate resin (A) having an intrinsic viscosity of 0.38 dL/g or less and a polyarylate resin (B) having an intrinsic viscosity of 0.40 to 0.65 dL/g, wherein a mass ratio of (A)/(B) is 90/10 to 10/90, and a difference in intrinsic viscosity between (A) and (B) is 0.3 dL/g or less.
<2> The composition according to <1>, wherein the polyarylate resin (B) has an intrinsic viscosity of 0.55 dL/g or less.
<3> The composition according to <1> or <2>, wherein the polycarbonate resin (A) has an intrinsic viscosity of 0.35 dL/g or less.
<4> The composition according to <1> or <2>, wherein the polycarbonate resin (A) has an intrinsic viscosity of 0.33 dL/g or less.
<5> The composition according to any one of <1> to <4>, wherein the difference in intrinsic viscosity between the polycarbonate resin (A) and the polyarylate resin (B) is 0.1 dL/g or more.
<6> The composition according to any one of <1> to <5>, wherein the polyarylate resin (B) contains a structural unit represented by formula (B-2).
Formula (B-2)

(In formula (B-2), R ⁸ each independently represents a fluorine atom, a chlorine atom, a bromine atom, an iodine atom, an alkyl group having 1 to 9 carbon atoms, an aryl group having 6 to 12 carbon atoms, an alkoxy group having 1 to 5 carbon atoms, an alkenyl group having 2 to 5 carbon atoms, or an aralkyl group having 7 to 17 carbon atoms; and q represents an integer of 0 to 5.)
<7> The composition according to any one of <1> to <6>, wherein the composition has a glass transition temperature of 150° C. or higher as measured by a differential scanning calorimeter.
<8> The composition according to any one of <1> to <7>, wherein the composition has a haze of 5.0% or less when molded into a thickness of 500 μm.
<9> The composition according to any one of <1> to <8>, further comprising an antioxidant (C).
<10> The composition according to <9>, wherein the antioxidant (C) includes a phosphorus-based antioxidant.
<11> The composition according to any one of <1> to <10>, further comprising an ester exchange inhibitor (D).
<12> A flat plate-like molded product formed from the composition according to any one of <1> to <11>.
<13> The flat plate-like molded product according to <12>, which is an extrusion molded product.
<14> The plate-like molded product according to <12> or <13>, having a thickness of 10 to 2000 μm.
<15> A method for producing a tabular molded product, comprising melt-extruding the composition according to any one of <1> to <11>.

The present invention makes it possible to provide a composition with excellent transparency, a flat plate-shaped molded body, and a method for manufacturing the flat plate-shaped molded body.

The present invention will be described in detail below. In this specification, the word "~" is used to mean that the numerical values before and after it are included as the lower and upper limits.

The composition of the present invention is characterized in that it contains a polycarbonate resin (A) having an intrinsic viscosity of 0.38 dL/g or less and a polyarylate resin (B) having an intrinsic viscosity of 0.4 to 0.65 dL/g, the mass ratio of (A)/(B) being 90/10 to 10/90, and the difference in intrinsic viscosity between (A) and (B) being 0.3 dL/g or less. By adopting such a constitution, a composition having excellent transparency can be obtained.
It has been found that when a composition containing a polycarbonate resin and a polyarylate resin is molded into a flat plate by extrusion molding, the obtained flat plate-shaped molded body may be whitened and have poor transparency. In this respect, the present invention solves the above problem by using a polycarbonate resin (A) having a low intrinsic viscosity and a polyarylate resin (B) having a limiting viscosity within a predetermined range, and by reducing the difference in the intrinsic viscosity between the two. That is, as described above, by adjusting the intrinsic viscosity, the compatibility of the polycarbonate resin (A) and the polyarylate resin (B) is increased, and whitening is successfully suppressed. In particular, the effect of the present invention is more effectively exhibited in extrusion molding, etc., where the cooling rate is slow during molding.
Furthermore, in the present invention, the compatibility between the polycarbonate resin (A) and the polyarylate resin (B) can be increased, so that a composition having a high Tg can be obtained by blending the polyarylate resin (B), which is a resin having a relatively high glass transition temperature (Tg), with the polycarbonate resin (A).

<Polycarbonate resin (A)>
The composition of the present invention contains a polycarbonate resin (A) having an intrinsic viscosity of 0.38 dL/g or less. By setting the intrinsic viscosity to 0.38 dL/g or less, the compatibility with the polyarylate resin (B) is improved, and the composition has excellent appearance and transparency.
The upper limit of the intrinsic viscosity of the polycarbonate resin (A) is preferably 0.35 dL/g or less, more preferably 0.33 dL/g or less. The lower limit of the intrinsic viscosity of the polycarbonate resin (A) is preferably 0.05 dL/g or more, more preferably 0.1 dL/g or more, even more preferably 0.2 dL/g or more, and may be 0.25 dL/g. By making the intrinsic viscosity equal to or more than the lower limit, the heat resistance of the composition tends to be further improved.
The intrinsic viscosity of the polycarbonate resin (A) is measured by the method described in the examples described below.

The weight average molecular weight of the polycarbonate resin (A) is preferably 10,000 or more, more preferably 15,000 or more. The upper limit of the weight average molecular weight of the polycarbonate resin (A) is preferably 100,000 or less, more preferably 80,000 or less, even more preferably 70,000 or less, and may be 50,000 or less, 40,000 or less, or 30,000 or less. By taking a value within the above range, a composition having excellent transparency and excellent heat resistance can be obtained.
The weight average molecular weight of the polycarbonate resin (A) is measured by the method described in the examples described later.

The viscosity average molecular weight of the polycarbonate resin (A) is preferably 8,000 or more, more preferably 10,000 or more. The upper limit of the viscosity average molecular weight of the polycarbonate resin (A) is preferably 80,000 or less, more preferably 50,000 or less, even more preferably 40,000 or less, and may be 30,000 or less, or 20,000 or less. By taking a value within the above range, a composition having excellent transparency and excellent heat resistance can be obtained.
The viscosity average molecular weight of the polycarbonate resin (A) is measured by the method described in the examples described later.

The glass transition temperature of the polycarbonate resin (A) measured by a differential scanning calorimeter is preferably 120° C. or higher, more preferably 135° C. or higher, and even more preferably 138° C. or higher. The upper limit of the glass transition temperature is preferably 160° C. or lower, and may be 150° C. or lower, or 145° C. or lower. By taking a value within the above range, a composition having superior heat resistance can be obtained.
The glass transition temperature of the polycarbonate resin (A) is measured by the method described in the examples described later.

式（Ａ－１）中、Ｘ^１は下記構造を表す。

Ｒ^５およびＲ^６は、アルキル基または水素原子であり、少なくとも一方がメチル基であることが好ましく、両方がメチル基であることがより好ましい。
式（Ａ－１）は下記式（Ａ－２）で表されることが好ましい。

The polycarbonate resin (A) is not particularly limited in type, but is preferably an aromatic polycarbonate resin, which can further improve compatibility with the polyarylate resin (B).
Preferred examples of the polycarbonate resin (A) include bisphenol A polycarbonate, bisphenol C polycarbonate, bisphenol AP polycarbonate, bisphenol Z polycarbonate, bisphenol TMC polycarbonate, and bisphenol E polycarbonate, and it is particularly preferred that the polycarbonate resin contains bisphenol A polycarbonate.
The bisphenol A polycarbonate resin refers to a resin having carbonate structural units derived from bisphenol A and its derivatives, and preferably has a structural unit represented by the following formula (A-1), in which * represents the bonding position with other structural units or terminal groups.

In formula (A-1), ^X1 represents the following structure.

^R5 and ^R6 each represent an alkyl group or a hydrogen atom, and it is preferable that at least one of them is a methyl group, and it is more preferable that both of them are methyl groups.
Formula (A-1) is preferably represented by the following formula (A-2).

The content of the structural unit represented by formula (A-1) in the bisphenol A polycarbonate resin is preferably 70 mol% or more, more preferably 80 mol% or more, and even more preferably 90 mol% or more, of all structural units excluding both ends. The upper limit is not particularly limited, and 100 mol% may be the structural unit represented by formula (A-1). Particularly preferred as the bisphenol A polycarbonate resin is a resin whose entire amount, excluding both ends, is substantially composed of structural units of formula (A-1). Here, substantially all structural units excluding both ends specifically means 99.0 mol% or more, preferably 99.5 mol% or more, and more preferably 99.9 mol% or more, of all structural units excluding both ends.
The bisphenol A polycarbonate resin may have other structural units than the carbonate structural units derived from bisphenol A and its derivatives. Examples of dihydroxy compounds constituting such other structural units include the aromatic dihydroxy compounds described in paragraph 0014 of JP-A-2018-154819, the contents of which are incorporated herein by reference.

The method for producing the polycarbonate resin (A) is not particularly limited, and any method can be used. Examples include interfacial polymerization, melt transesterification, pyridine method, ring-opening polymerization of cyclic carbonate compounds, and solid-phase transesterification of prepolymers.

The composition of the present invention preferably contains polycarbonate resin (A) in an amount of 25 to 75% by mass, and more preferably in an amount of 28 to 72% by mass.

<Polyarylate resin (B)>
The composition of the present invention contains a polyarylate resin (B) having an intrinsic viscosity of 0.40 to 0.65 dL/g. By making the intrinsic viscosity equal to or more than the lower limit, the heat resistance of the resulting composition is improved, and by making the intrinsic viscosity equal to or less than the upper limit, the compatibility with the polycarbonate resin (A) is improved and whitening of the composition and molded articles is suppressed.
The intrinsic viscosity of the polyarylate resin (B) is preferably 0.42 dL/g or more, and may be 0.45 dL/g or more. The intrinsic viscosity of the polyarylate resin (B) is preferably 0.55 dL/g or less, more preferably 0.52 dL/g or less, and even more preferably 0.50 dL/g or less. When two or more kinds of polyarylate resins (B) are blended, the intrinsic viscosity is the intrinsic viscosity of the mixture. The same applies to other physical properties and other resins (such as polycarbonate resins).
The intrinsic viscosity of the polyarylate resin (B) is measured according to the description in the Examples section described later.

The weight average molecular weight of the polyarylate resin (B) is preferably 25,000 or more, more preferably 30,000 or more, even more preferably 35,000 or more, even more preferably 37,000 or more, and may be 40,000 or more. By making it equal to or more than the lower limit, a composition having excellent mechanical strength such as impact properties and bending properties can be obtained. In addition, the upper limit of the weight average molecular weight of the polyarylate resin (B) is preferably 80,000 or less, more preferably 60,000 or less, and even more preferably 50,000 or less. By making it equal to or less than the upper limit, a composition having excellent moldability can be obtained.
The weight average molecular weight of the polyarylate resin (B) is measured by the method described in the examples described later.

The glass transition temperature of the polyarylate resin (B) measured by a differential scanning calorimeter is preferably more than 160° C., more preferably 170° C. or more, even more preferably 180° C. or more, and even more preferably 190° C. or more. The upper limit of the glass transition temperature is preferably 250° C. or less, and may be 240° C. or less, 230° C. or less, 220° C. or less, or 200° C. or less. By setting it to the above lower limit or more, the heat resistance of the obtained composition can be further improved, and by setting it to the above upper limit or less, the melt viscosity can be set to a more appropriate range.
The glass transition temperature of the polyarylate resin (B) is measured by the method described in the examples below.

The polyarylate resin (B) used in the present invention is preferably an aromatic polyester composed of structural units derived from an aromatic dicarboxylic acid and structural units derived from a bisphenol.
Examples of aromatic dicarboxylic acids include terephthalic acid, isophthalic acid, 1,4-naphthalenedicarboxylic acid, 1,5-naphthalenedicarboxylic acid, 2,6-naphthalenedicarboxylic acid, benzophenone dicarboxylic acid, 4,4'-diphenyldicarboxylic acid, 3,3'-diphenyldicarboxylic acid, and 4,4'-diphenylether dicarboxylic acid, with terephthalic acid and isophthalic acid being more preferred.
Examples of bisphenols include 2,2-bis(4-hydroxyphenyl)propane, 2,2-bis(4-hydroxy-3,5-dimethylphenyl)propane, 2,2-bis(4-hydroxy-3,5-dibromophenyl)propane, 2,2-bis(4-hydroxy-3,5-dichlorophenyl)propane, 4,4'-dihydroxydiphenyl sulfone, 4,4'-dihydroxydiphenyl ether, 4,4'-dihydroxydiphenyl sulfide, 4,4'-dihydroxydiphenyl ketone, 4,4'-dihydroxydiphenylmethane, 1,1-bis(4-hydroxyphenyl)cyclohexane, 1,1-bis(4-hydroxyphenyl)-1-phenylethane, and 1,1-bis(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane. These compounds may be used alone or in combination of two or more.

式（Ｂ－１）中、Ｘ^８は下記構造を表す。

Ｒ^５およびＲ^６は、アルキル基または水素原子であり、少なくとも一方がメチル基であることが好ましく、両方がメチル基であることがより好ましい。
式（Ｂ－１）で表される構成単位は、例えば、ビスフェノールＡおよびその誘導体の少なくとも１種と、テレフタル酸およびイソフタル酸、ならびに、それらの誘導体の少なくとも１種とから形成される。テレフタル酸とイソフタル酸のモル比率は、４０～６０：６０～４０であることが好ましい。 More specifically, the polyarylate resin (B) preferably contains a structural unit represented by the following formula (B-1) and/or a structural unit represented by the following formula (B-2), in which * represents a bonding position with other structural units or terminal groups.
Formula (B-1)

In formula (B-1), ^X8 represents the following structure.

^R5 and ^R6 each represent an alkyl group or a hydrogen atom, and it is preferable that at least one of them is a methyl group, and it is more preferable that both of them are methyl groups.
The structural unit represented by formula (B-1) is formed, for example, from at least one of bisphenol A and its derivatives, and at least one of terephthalic acid, isophthalic acid, and their derivatives. The molar ratio of terephthalic acid to isophthalic acid is preferably 40-60:60-40.

式（Ｂ－２）中、Ｒ^８は、それぞれ独立に、フッ素原子、塩素原子、臭素原子、ヨウ素原子、炭素原子数１～９（好ましくは１～３）のアルキル基、炭素原子数６～１２（好ましくは６～１０）のアリール基、炭素原子数１～５（好ましくは１～３）のアルコキシ基、炭素原子数２～５（好ましくは２または３）のアルケニル基または炭素原子数７～１７（好ましくは７～１１）のアラルキル基を表す。ｑは０～５の整数を表し、１～３の整数が好ましい。
Ｒ^８は、それぞれ独立に、炭素原子数１～９（好ましくは１～３）のアルキル基が好ましく、メチル基がより好ましい。 Formula (B-2)

In formula (B-2), R ^8s each independently represent a fluorine atom, a chlorine atom, a bromine atom, an iodine atom, an alkyl group having 1 to 9 carbon atoms (preferably 1 to 3), an aryl group having 6 to 12 carbon atoms (preferably 6 to 10), an alkoxy group having 1 to 5 carbon atoms (preferably 1 to 3), an alkenyl group having 2 to 5 carbon atoms (preferably 2 or 3), or an aralkyl group having 7 to 17 carbon atoms (preferably 7 to 11). q represents an integer of 0 to 5, preferably an integer of 1 to 3.
Each R ⁸ is independently preferably an alkyl group having 1 to 9 carbon atoms (preferably 1 to 3 carbon atoms), more preferably a methyl group.

式（Ｂ－３）中、Ｒ^８は式（Ｂ－２）におけるＲ^８と同義であり、好ましい範囲も同様である。
式（Ｂ－２）で表される構成単位は、例えば、ビスフェノールＴＭＣおよびその誘導体の少なくとも１種と、テレフタル酸およびイソフタル酸、ならびに、それらの誘導体の少なくとも１種とから形成される。テレフタル酸とイソフタル酸のモル比率は、４０～６０：６０～４０であることが好ましい。 The constitutional unit represented by formula (B-2) is preferably a constitutional unit represented by formula (B-3).
Formula (B-3)

In formula (B-3), R ⁸ has the same meaning as R ⁸ in formula (B-2), and the preferred range is also the same.
The structural unit represented by formula (B-2) is formed, for example, from at least one of bisphenol TMC and its derivatives, and at least one of terephthalic acid, isophthalic acid, and their derivatives. The molar ratio of terephthalic acid to isophthalic acid is preferably 40-60:60-40.

The first embodiment of the polyarylate resin (B) used in the present invention is an embodiment containing 90 mol % or more of the structural unit represented by formula (B-1) of all structural units excluding both ends. The composition containing the polyarylate resin of the first embodiment is particularly excellent in balance between fluidity and heat resistance, and can be suitably used for applications in which fluidity and heat resistance are particularly required.
The second embodiment of the polyarylate resin (B) used in the present invention is an embodiment containing the structural unit represented by formula (B-1) and the structural unit represented by formula (B-2) in a molar ratio of 90 to 40: 10 to 60, more preferably 90 to 51: 10 to 49, and more preferably 85 to 55: 15 to 45. The structural unit represented by formula (B-1) and the structural unit represented by formula (B-2) may be contained in the same polyarylate resin, or may be a blend of a polyarylate resin containing a structural unit represented by formula (B-1) and a polyarylate resin containing a structural unit represented by formula (B-2). In addition, in the second embodiment, it is more preferable that the polyarylate resin (B) used in the present invention contains the structural unit represented by formula (B-1) and the structural unit represented by formula (B-2) in a total of 90 mol% or more of all structural units excluding both ends. A composition containing the polyarylate resin of the second embodiment has excellent compatibility with polycarbonate resins, and therefore can be suitably used in applications where transparency is particularly required.

<Relationship between polycarbonate resin (A) and polyarylate resin (B)>
In the composition of the present invention, the mass ratio of the polycarbonate resin (A) to the polyarylate resin (B) is 90/10 to 10/90. The mass ratio is preferably 80/20 to 20/80, more preferably 75/25 to 25/75, even more preferably 72/28 to 28/72, even more preferably 65/35 to 35/65, and even more preferably 65/35 to 45/55.
Furthermore, when it is desired to lower the melt viscosity of the composition, the mass ratio is preferably 75/25 to 65/35, and when it is desired to improve the heat resistance of the composition, the mass ratio is preferably 35/65 to 25/75.

In the composition of the present invention, the difference in intrinsic viscosity between the polycarbonate resin (A) and the polyarylate resin (B) is 0.3 dL/g or less. The lower limit of the difference in intrinsic viscosity is preferably 0.1 dL/g or more, more preferably 0.12 L/g or more, and may be 0.15 L/g or more, or 0.17 dL/g or more. The upper limit of the difference in intrinsic viscosity is preferably 0.25 dL/g or less, more preferably 0.22 dL/g or less, and even more preferably 0.20 dL/g or less. By keeping it within the above range, a composition with better transparency can be obtained.
In the composition of the present invention, the total content of the polycarbonate resin (A) and the polyarylate resin (B) is preferably 90% by mass or more, more preferably 95% by mass or more, even more preferably 97% by mass or more, even more preferably 98% by mass or more, and even more preferably 99% by mass or more of the composition. By setting it in such a range, the effects of the present invention tend to be more effectively exhibited.
The composition of the present invention may contain only one type of polycarbonate resin (A), or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.
The composition of the present invention may contain only one type of polyarylate resin (B), or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

<Antioxidant (C)>
The composition of the present invention preferably contains an antioxidant (C).
The antioxidant (C) may be a phenol-based antioxidant, an amine-based antioxidant, a phosphorus-based antioxidant, a thioether-based antioxidant, etc., and is preferably at least one of a phosphorus-based antioxidant (more preferably a phosphite-based antioxidant) and a phenol-based antioxidant (more preferably a hindered phenol-based antioxidant), and is particularly preferably a phosphorus-based antioxidant. It is also preferable to use a phosphorus-based antioxidant and a phenol-based antioxidant in combination.

The phosphorus-based antioxidant is not particularly limited as long as it is an antioxidant containing a phosphorus atom.
Specific examples of phosphorus-based antioxidants include phosphorus oxoacids such as phosphoric acid, phosphonic acid, phosphorous acid, phosphinic acid, and polyphosphoric acid; metal acid pyrophosphates such as sodium acid pyrophosphate, potassium acid pyrophosphate, and calcium acid pyrophosphate; phosphates of Group 1 or Group 2B metals such as potassium phosphate, sodium phosphate, cesium phosphate, and zinc phosphate; phosphate compounds, phosphite compounds, and phosphonite compounds, with phosphite compounds being particularly preferred. By selecting a phosphite compound, a tabular molded product having higher discoloration resistance and continuous productivity can be obtained.
For the phosphorus-based antioxidant, the description in paragraphs 0058 to 0064 of JP 2018-090677 A can be referred to, the contents of which are incorporated herein by reference.

（式（１）中、Ｒ^１およびＲ^２はそれぞれ独立に、炭素原子数１～３０のアルキル基または炭素原子数６～３０のアリール基を表す。）

（式（２）中、Ｒ^３～Ｒ^７は、それぞれ独立に、水素原子、炭素原子数６～２０のアリール基または炭素原子数１～２０のアルキル基を表す。）
上記式（１）中、Ｒ^１、Ｒ^２で表されるアルキル基は、それぞれ独立に、炭素原子数１～１０の直鎖または分岐のアルキル基であることが好ましい。Ｒ^１、Ｒ^２がアリール基である場合、以下の一般式（１－ａ）、（１－ｂ）、または（１－ｃ）のいずれかで表されるアリール基が好ましい。

（式（１－ａ）中、Ｒ^Ａは、それぞれ独立に、炭素原子数１～１０のアルキル基を表す。式（１－ｂ）中、Ｒ^Ｂは、それぞれ独立に、炭素原子数１～１０のアルキル基を表す。）
式（１）で表される化合物の中でも、特にビス（２，６－ジ－ｔｅｒｔ－ブチル－４－メチルフェニル）ペンタエリスリトールジホスファイト、ビス（２，４－ジクミルフェニル）ペンタエリスリトールジホスファイト）などが好適に使用できる。
式（２）で表される化合物の中でも、特にトリス（２，４－ジ－ｔｅｒｔ－ブチルフェニル）ホスファイトなどが好適に使用できる。 The phosphorus-based antioxidant used in the present invention is preferably a phosphite compound represented by the following formula (1) or (2).

(In formula (1), R ¹ and R ² each independently represent an alkyl group having 1 to 30 carbon atoms or an aryl group having 6 to 30 carbon atoms.)

(In formula (2), R ³ to R ⁷ each independently represent a hydrogen atom, an aryl group having 6 to 20 carbon atoms, or an alkyl group having 1 to 20 carbon atoms.)
In the above formula (1), the alkyl groups represented by R ¹ and R ² are preferably each independently a linear or branched alkyl group having 1 to 10 carbon atoms. When R ¹ and R ² are aryl groups, they are preferably aryl groups represented by any one of the following general formulas (1-a), (1-b), or (1-c).

(In formula (1-a), R ^A each independently represents an alkyl group having 1 to 10 carbon atoms. In formula (1-b), R ^B each independently represents an alkyl group having 1 to 10 carbon atoms.)
Among the compounds represented by formula (1), bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite, bis(2,4-dicumylphenyl)pentaerythritol diphosphite, and the like can be particularly suitably used.
Among the compounds represented by formula (2), tris(2,4-di-tert-butylphenyl)phosphite is particularly suitable.

Examples of phenol-based antioxidants include hindered phenol-based antioxidants. As such phenol-based antioxidants, the phenol-based antioxidants described in paragraph 0041 of JP-A-2019-002023 and the phenol-based antioxidants described in paragraphs 0033 to 0034 of JP-A-2019-056035 are preferably used, the contents of which are incorporated herein by reference.

The content of the antioxidant (C) in the composition, when contained, is preferably 0.005 parts by mass or more, more preferably 0.007 parts by mass or more, and even more preferably 0.01 parts by mass or more, relative to 100 parts by mass of the resin component (meaning the total of the polycarbonate resin (A) and the polyarylate resin (B)). The upper limit of the content of the antioxidant (C) is preferably 4 parts by mass or less, more preferably 1 part by mass or less, even more preferably 0.5 parts by mass or less, and even more preferably 0.1 parts by mass or less, relative to 100 parts by mass of the resin component.
By setting the content of the antioxidant (C) to 0.005 parts by mass or more, the transparency tends to be further improved, and by setting the content of the antioxidant (C) to 4 parts by mass or less, the moist heat stability tends to be further improved.
When a phosphorus-based antioxidant and a phenol-based antioxidant (preferably a hindered phenol-based antioxidant) are used in combination as the antioxidant (C), the contents thereof are preferably in the range of 0.001 to 0.2 parts by mass of the phosphorus-based antioxidant and 0.001 to 0.2 parts by mass of the phenol-based antioxidant per 100 parts by mass of the resin component.
As described above, the antioxidant (C) may be used alone or in combination of two or more. When two or more types are used, it is preferable that the total amount is in the above range.

<Interesterification inhibitor (D)>
The composition of the present invention preferably contains an ester exchange inhibitor (D).
The transesterification inhibitors include phosphorus-based transesterification inhibitors and sulfur-based transesterification inhibitors.
Examples of phosphorus-based ester exchange inhibitors include phosphorous acid, phosphoric acid, phosphonous acid, phosphonic acid, and esters thereof, and alkyl phosphites are particularly suitable.
As the transesterification inhibitor, the descriptions in paragraphs 0035 to 0039 of WO 2015/190162, paragraph 0037 of JP-A 2019-002023, and paragraph 0041 of JP-A 2018-199745 can be referred to, and the contents of these are incorporated herein.

The content of the transesterification inhibitor (D) in the composition, when contained, is preferably 0.001 parts by mass or more, more preferably 0.005 parts by mass or more, and even more preferably 0.007 parts by mass or more, relative to 100 parts by mass of the resin component. The upper limit of the content of the transesterification inhibitor (D) is preferably 1.0 parts by mass or less, more preferably 0.5 parts by mass or less, even more preferably 0.3 parts by mass or less, and even more preferably 0.1 parts by mass or less, relative to 100 parts by mass of the resin component. By setting the content of the transesterification inhibitor (D) within the above range, the molecular weight reduction of the composition can be more effectively suppressed.
The transesterification inhibitor (D) may be contained in one kind or in two or more kinds. When two or more kinds are contained, it is preferable that the total amount is in the above range.

<Release Agent (E)>
The composition of the present invention preferably contains a release agent (E).
The release agent (E) may be at least one compound selected from the group consisting of aliphatic carboxylic acids, esters of aliphatic carboxylic acids and alcohols, aliphatic hydrocarbon compounds having a number average molecular weight of 200 to 15,000, and polysiloxane-based silicone oils, and is preferably an ester of aliphatic carboxylic acids and alcohols.
Specific examples of esters of aliphatic carboxylic acids and alcohols include beeswax (a mixture containing myricyl palmitate as a main component), stearyl stearate, behenyl behenate, stearyl behenate, glycerin monopalmitate, glycerin monostearate, glycerin distearate, glycerin tristearate, pentaerythritol monopalmitate, pentaerythritol monostearate, pentaerythritol distearate, pentaerythritol tristearate, and pentaerythritol tetrastearate.
In addition, as the release agent (E), the release agents described in paragraph 0032 of JP-A-2017-226848 and paragraph 0056 of JP-A-2018-199745 can be used, the contents of which are incorporated herein by reference.

The content of the release agent (E) in the composition, when contained, is preferably 0.001 part by mass or more, more preferably 0.005 part by mass or more, and is preferably 2 parts by mass or less, more preferably 1 part by mass or less, and even more preferably 0.5 parts by mass or less, relative to 100 parts by mass of the resin component.
The release agent (E) may be used alone or in combination of two or more. When two or more types are used, it is preferable that the total amount is within the above range.

<Other ingredients>
In addition to the above, the composition may contain other thermoplastic resins, heat stabilizers, flame retardants, flame retardant assistants, ultraviolet absorbers, colorants, antistatic agents, fluorescent brighteners, antifogging agents, flow improvers, plasticizers, dispersants, antibacterial agents, antiblocking agents, impact improvers, sliding improvers, hue improvers, acid trapping agents, etc. These components may be used alone or in combination of two or more.
When contained, the total amount of the other components is preferably 0.001 to 5 mass %, more preferably 0.001 to 2 mass %, and even more preferably 0.01 to 1 mass % of the composition. Anti-blocking refers to the effect of suppressing adhesion between films, and can be achieved by adding an anti-blocking agent, etc.

<Physical Properties of Composition>
The composition of the present invention preferably has a shear viscosity at 300°C and a shear rate of 122 sec ^-1 (such a value is referred to as the "melt viscosity" in the present invention) of 3,500 Pa·s or less, more preferably 900 Pa·s or less, and even more preferably 700 Pa·s or less. The lower limit of the melt viscosity is preferably 50 Pa·s or more, more preferably 100 Pa·s or more, and may even be 160 Pa·s or more, or 200 Pa·s or more. By taking a value within the above range, a composition having excellent moldability by melt extrusion can be obtained.
The melt viscosity is measured by the method described in the Examples below.

The composition of the present invention, when molded to a thickness of 500 μm, preferably has a total light transmittance of 87% or more, more preferably 88% or more, and even more preferably 89% or more. The upper limit of the total light transmittance is not particularly limited, but for example, 94% or less is practical.
The total light transmittance is measured based on the method described in the examples below.

The composition of the present invention preferably has a haze of 5.0% or less, more preferably 4.0% or less, even more preferably 3.0% or less, even more preferably 2.0% or less, even more preferably 1.0% or less, and even more preferably 0.8% or less when molded to a thickness of 500 μm. There is no particular lower limit, but even if it is 0.1% or more, the performance requirements are sufficiently met.
The haze is measured based on the method described in the examples described below.

The composition of the present invention preferably has a glass transition temperature measured by a differential scanning calorimeter of 150° C. or higher. The polyarylate resin (B) has a relatively high glass transition temperature, and in the present invention, has excellent compatibility with the polycarbonate resin (A), so that the glass transition temperature of the composition can be increased.
The glass transition temperature may be 155° C. or higher, and may further be 160° C. or higher, 170° C. or higher, or 175° C. or higher. There is no particular upper limit to the glass transition temperature, but for example, 190° C. or lower is practical.
The glass transition temperature (Tg) is measured by the method described in the Examples section below.

The composition of the present invention may contain a monofunctional phenol compound. Examples of monofunctional phenol compounds include dibutylhydroxytoluene, and are mainly derived from unreacted materials derived from the raw materials of the polycarbonate resin (A) and the polyarylate resin (B), and decomposition products of the antioxidant (C), etc. In the present invention, the total amount of the monofunctional phenol compound is preferably more than 10,000 ppm by mass of the composition, and more preferably more than 10,000 ppm by mass but less than 1 part by mass. By setting the amount in such a range, the effects of the present invention tend to be more effectively exhibited.

<Production method of composition>
The method for producing the composition of the present invention is not limited, and a wide variety of known methods for producing compositions can be adopted. Examples of the method include a method in which the polycarbonate resin (A), the polyarylate resin (B), and other components to be blended as necessary are premixed using various mixers such as a tumbler or a Henschel mixer, and then melt-kneaded using a mixer such as a Banbury mixer, a roll, a Brabender, a single-screw kneading extruder, a twin-screw kneading extruder, or a kneader.
The melt-kneading temperature is not particularly limited, but is usually in the range of 240 to 360°C.
The melt-kneaded composition is, for example, strand-cut to obtain pellets. The pellets thus obtained are, for example, extruded by an extruder to produce a plate-shaped molded product (for example, a film-shaped or sheet-shaped molded product). Also, molded products of any shape can be produced by injection molding using an injection molding machine.

The flat-plate molded article of the present invention is preferably produced, for example, by melt extruding the composition of the present invention. That is, one embodiment of the flat-plate molded article of the present invention is an extrusion molded product. In extrusion molding, the cooling rate is relatively slow, and since it is an open molding method, transparency is easily impaired. In the present invention, by using a specified composition, a flat-plate molded article with excellent transparency can be obtained even by extrusion molding.

<Molded body>
The molded article of the present invention is molded from the composition of the present invention. The molded article of the present invention is preferably used for electrical and electronic equipment, office automation equipment, mobile information terminals, machine parts, home appliances, vehicle parts, various containers, lighting equipment, and other parts. Among these, it is particularly preferably used for electrical and electronic equipment, office automation equipment, information terminal equipment, and home appliance housings, lighting equipment, and vehicle parts (particularly vehicle interior parts), surface films for smartphones and touch panels, optical materials, and optical disks. In particular, the molded article of the present invention is suitable for use as a sensor for a touch panel.

As an embodiment of the molded product of the present invention, a flat molded body is exemplified. In particular, in the present invention, it is preferably used as a transparent flat molded body for high heat resistance applications. More specifically, it can be used as a plate-shaped molded body for transparent electrode substrates. Here, the transparent electrode is a transparent substrate having a transparent electrode layer disposed on one or both surfaces. An additional layer may be present between the transparent substrate and the transparent electrode layer. The plate-shaped molded body of the present invention can be used as the transparent substrate in this transparent electrode. It can also be preferably used as a protective film for protecting products for high heat resistance applications.
The thickness of the plate-shaped molded product formed from the composition of the present invention is not particularly limited, but is preferably 10 μm or more, more preferably 25 μm or more, and even more preferably 50 μm or more. The upper limit is preferably 2,000 μm or less, more preferably 1,000 μm or less, and even more preferably 750 μm or less.

The present invention will be explained in more detail below with reference to examples. The materials, amounts used, ratios, processing contents, processing procedures, etc. shown in the following examples can be changed as appropriate without departing from the spirit of the present invention. Therefore, the scope of the present invention is not limited to the specific examples shown below.

<Ingredients>
Polycarbonate resin (A)
A1: Aromatic polycarbonate resin obtained by interfacial polymerization using bisphenol A as a starting material, manufactured by Mitsubishi Engineering Plastics Corporation, H-7000F, weight average molecular weight: 24,900, viscosity average molecular weight: 14,000, Tg: 141°C, intrinsic viscosity: 0.3 dL/g
A2: Aromatic polycarbonate resin obtained by interfacial polymerization using bisphenol A as a starting material, manufactured by Mitsubishi Engineering Plastics Corporation, L-1000F, weight average molecular weight: 16,700, viscosity average molecular weight: 10,800, Tg: 136°C, intrinsic viscosity: 0.24 dL/g
A3: Aromatic polycarbonate resin obtained by interfacial polymerization using bisphenol A as a starting material, manufactured by Mitsubishi Engineering Plastics Corporation, S-3000F, weight average molecular weight: 41,300, viscosity average molecular weight: 21,000, Tg: 148°C, intrinsic viscosity: 0.43 dL/g

Polyarylate resin (B)
B1: U-Powder D type, manufactured by Unitika Ltd., dicarboxylic acid component: terephthalic acid/isophthalic acid = 50/50 mol%, bisphenol component: bisphenol A = 100 mol%
Weight average molecular weight 63,000, intrinsic viscosity 0.65 dL/g, Tg: 201°C
B2: U-Powder L type, manufactured by Unitika Ltd., dicarboxylic acid component: terephthalic acid/isophthalic acid = 50/50 mol%, bisphenol component: bisphenol A = 100 mol%
Weight average molecular weight 40,800, intrinsic viscosity 0.48 dL/g, Tg: 195°C
B3: U-Powder T-240AF, manufactured by Unitika Ltd., dicarboxylic acid component: terephthalic acid/isophthalic acid=50/50 mol%, bisphenol component: bisphenol A/bisphenol TMC=60/40 mol%
Weight average molecular weight 38,000, intrinsic viscosity 0.43 dL/g, Tg: 224°C
B4: Unitika Ltd., a 1:1 (mass ratio) blend of U-Powder T-240AF and U-Powder L type, weight average molecular weight 39,400, intrinsic viscosity 0.46 dL/g, Tg: 210°C

Antioxidant (C)
C1: Tris(2,4-di-tert-butylphenyl)phosphite, phosphorus-based antioxidant, manufactured by ADEKA Corporation, Adeka STAB 2112
C2: Bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite, phosphorus-based antioxidant, manufactured by ADEKA Corporation, Adeka STAB PEP-36
C3: tetrakis[3-(3',5'-di-tert-butyl-4-hydroxyphenyl)propionic acid]pentaerythritol, a hindered phenol-based antioxidant, manufactured by ADEKA Corporation, Adeka STAB AO-60
C4: Bis(2,4-dicumylphenyl)pentaerythritol diphosphite), manufactured by Dover Chemical Company, Doverphos S-9228PC

・Esterification inhibitor (D)
D1: Octadecyl phosphite, manufactured by ADEKA Corporation, AX-71

Release agent (E)
E1: Glycerin monostearate, Riken Vitamin Co., Ltd., Rikemal S-100A

Examples 1 to 7, Comparative Examples 1 and 2
The above components were weighed out so as to obtain the amounts shown in Table 1 or Table 2. The mixture was then mixed in a tumbler for 15 minutes, melt-kneaded in a vented twin-screw extruder at a cylinder temperature of 320° C., and pellets were obtained by strand cutting.
The twin-screw extruder used was a "TEX30α" with a screw diameter of 32 mm manufactured by Japan Steel Works, Ltd.

The resulting pellets were used to produce a film in the following manner.
The pellets obtained above were dried at 120°C for 5 hours, and then extruded in a molten state using a T-die melt extruder consisting of a vented twin-screw extruder with a barrel diameter of 32 mm and a screw L/D of 31.5 (manufactured by Japan Steel Works, Ltd., "TEX30α") at a discharge rate of 10 kg/h and a screw rotation speed of 63 rpm, and then cooled and solidified to produce a film with a thickness of 500 μm. The cylinder and die head temperature was 280°C.

The melt viscosity and Tg of the resulting composition (pellets) were measured. The total light transmittance and haze of the resulting film were also measured.

<Method for measuring weight average molecular weight>
The weight average molecular weight (Mw) of the polycarbonate resin (A) and the polyarylate resin (B) was measured by gel permeation chromatography as follows.
The gel permeation chromatography apparatus used was an LC-20AD system (manufactured by Shimadzu Corporation), and an LF-804 (manufactured by Shodex Corporation) was connected as the column. The column temperature was 40° C. The detector used was an RID-10A (manufactured by Shimadzu Corporation) RI detector. Chloroform was used as the eluent, and a calibration curve was created using standard polystyrene (manufactured by Tosoh Corporation).
If the above-mentioned gel permeation chromatography device, column, and detector are difficult to obtain, measurement can be performed using other devices having equivalent performance.

<Measurement of Glass Transition Temperature (Tg)>
The glass transition temperatures (Tg) of the polycarbonate resin (A), the polyarylate resin (B), and the composition were measured by performing two cycles of heating and cooling under the following DSC measurement conditions, and measuring the glass transition temperature during the second heating cycle.
The starting glass transition temperature was determined as the intersection point of a straight line extending the low-temperature side baseline to the high-temperature side and a tangent to the inflection point, the ending glass transition temperature was determined as the intersection point of a straight line extending the high-temperature side baseline to the low-temperature side and a tangent to the inflection point, and the midpoint between the starting glass transition temperature and the ending glass transition temperature was determined as the glass transition temperature (Tg). Measurement starting temperature: 30°C, heating rate: 10°C/min, final temperature: 250°C, heating rate: 20°C/min.
The measurement was performed using a differential scanning calorimeter (DSC, Hitachi High-Tech Science Corporation, "DSC7020").

<Method of measuring intrinsic viscosity and viscosity average molecular weight>
The intrinsic viscosity [η] (unit: dL/g) of the polycarbonate resin (A) and the polyarylate resin (B) was measured using methylene chloride as a solvent. The temperature was set at 25°C. The specific viscosity [η _sp ] at each solution concentration [C] (g/dL) was measured using an Ubbelohde viscometer. The intrinsic viscosity was calculated from the obtained specific viscosity value and concentration according to the following formula.

The viscosity average molecular weight [Mv] was calculated from Schnell's viscosity formula, ie, η=1.23×10 ⁻⁴ Mv ^0.83 .

<Measurement of Melt Viscosity of Composition>
The composition (the obtained pellets) was dried for 5 hours at 120° C. Then, using a capillary rheometer, the resin was extruded from a nozzle hole (orifice) of 10 mm length × 1.0 mm diameter at 300° C. The shear viscosity (unit: Pa s) at this time was measured at a shear rate of 122 sec ⁻¹ and was taken as the melt viscosity.
The capillary rheometer used was "Capillograph 1B" (product name) manufactured by Toyo Seiki Seisakusho, Ltd.

<Measurement of total light transmittance and haze>
The total light transmittance (%) and haze (%) of the 500 μm-thick film obtained above were measured using a haze meter in accordance with JIS-K-7361 and JIS-K-7136 under conditions of a D65 light source and a 10° visual field.
The haze meter used was "HM-150" (product name) manufactured by Murakami Color Research Laboratory.

Claims (14)

A composition comprising a polycarbonate resin (A) having an intrinsic viscosity of 0.35 dL/g or less and a polyarylate resin (B) having an intrinsic viscosity of 0.40 to 0.65 dL/g, wherein the mass ratio of (A)/(B) is 90/10 to 10/90, and the difference in intrinsic viscosity between (A) and (B) is 0.3 dL/g or less ,
A composition, wherein the polycarbonate resin (A) is a bisphenol A type polycarbonate, and the total content of the polycarbonate resin (A) and the polyarylate resin (B) is 95 mass% or more of the composition. The composition according to claim 1, wherein the polyarylate resin (B) has an intrinsic viscosity of 0.55 dL/g or less. The composition according to claim 1 or 2, wherein the intrinsic viscosity of the polycarbonate resin (A) is 0.33 dL/g or less. The composition according to any one of claims 1 to 3 , wherein the difference in intrinsic viscosity between the polycarbonate resin (A) and the polyarylate resin (B) is 0.1 dL/g or more. The composition according to any one of claims 1 to 4 , wherein the polyarylate resin (B) contains a structural unit represented by formula (B-2).
Formula (B-2)

(In formula (B-2), R ⁸ each independently represents a fluorine atom, a chlorine atom, a bromine atom, an iodine atom, an alkyl group having 1 to 9 carbon atoms, an aryl group having 6 to 12 carbon atoms, an alkoxy group having 1 to 5 carbon atoms, an alkenyl group having 2 to 5 carbon atoms, or an aralkyl group having 7 to 17 carbon atoms; and q represents an integer of 0 to 5.) The composition according to any one of claims 1 to 5 , wherein the composition has a glass transition temperature of 150°C or higher as measured by a differential scanning calorimeter. The composition according to any one of claims 1 to 6 , wherein the composition has a haze of 5.0% or less when molded to a thickness of 500 µm. The composition according to any one of claims 1 to 7 , further comprising an antioxidant (C). The composition of claim 8 , wherein the antioxidant (C) comprises a phosphorus-based antioxidant. The composition according to any one of claims 1 to 9 , further comprising an ester exchange inhibitor (D). A flat molded article formed from the composition according to any one of claims 1 to 10 . The flat plate-like molded article according to claim 11 , which is an extrusion molded product. The plate-like molded article according to claim 11 or 12 , having a thickness of 10 to 2000 μm. A method for producing a tabular molded article, comprising melt-extruding the composition according to any one of claims 1 to 10 .