JP7560982B2 - Coenzyme Q10-containing water-soluble composition - Google Patents

Description

The present invention relates to a water-soluble composition containing Coenzyme Q10.
In detail, the present invention relates to a water-soluble composition containing coenzyme Q10, which contains fat-soluble coenzyme Q10 and has excellent long-term storage stability, i.e., when added to an aqueous liquid, particularly an aqueous solution containing collagen, coenzyme Q10 does not separate, precipitate, deposit or float to the surface, even in the aqueous composition thus produced in which collagen is present at a high concentration.

In recent years, with the growth of the health food market, product differentiation has progressed, the functional ingredients used have become more diverse, and many products with high functional ingredient content have been developed. Many fat-soluble functional ingredients, such as coenzyme Q10, play essential or important roles in the body, and there is great demand for their use in health foods.

Coenzyme Q10, also known as ubidecarenone or coenzyme Q10, is a type of coenzyme present in higher animals. Coenzyme Q10 is known as a vitamin-like substance that not only has biological activity as a coenzyme, but also has the effect of improving oxygen utilization efficiency. Coenzyme Q10 has effects such as energy production and antioxidant properties, and is said to be involved in various health functions. It is clinically used to improve the symptoms of angina pectoris, heart failure, ischemic heart disease, and muscular dystrophy, and is said to be effective against high blood pressure, arteriosclerosis, heart disease, diabetes, cancer, etc., and has also been reported to be effective in recovering from fatigue and restoring motor function. As such, coenzyme Q10 has high physiological activity and is present in the body, making it a highly safe substance.

However, since coenzyme Q10 is a lipophilic solid with a low melting point, it is poorly soluble in water, unstable to light and heat, and highly crystalline, so it is generally difficult to formulate it by emulsification. Even if an emulsion composition is prepared, separation, precipitation, deposition, or floating due to recrystallization of coenzyme Q10 is likely to occur, and there is a problem that the long-term storage stability is low.

Therefore, it is necessary to improve the emulsion stability of coenzyme Q10 in aqueous compositions, and several techniques have been proposed to date.

Patent Document 1 discloses an aqueous liquid preparation that maintains homogeneity for a long period of time, which is obtained by stirring polyglycerol fatty acid ester, glycerin and coenzyme Q10 and then emulsifying it with a high-pressure homogenizer.

Patent Document 2 discloses a water-soluble composition that has excellent heat, salt and acid resistance and contains coenzyme Q10, an ester of polyglycerol with an average degree of polymerization of 10 and a fatty acid with 18 carbon atoms, an ester of polyglycerol with an average degree of polymerization of 3 to 6 and a fatty acid with 18 carbon atoms, and water.

Patent Document 3 discloses an oil-in-water emulsion with excellent heat, acid and alcohol resistance, which is obtained by using an emulsifier composition containing a polyglycerol fatty acid ester, a sucrose fatty acid ester and lecithin, and coenzyme Q10.

Patent Document 4 discloses a food additive composition that contains coenzyme Q10 and a polyglycerol fatty acid ester consisting of a polyglycerol containing no glycerol and 3% or less diglycerol and fatty acids, and that can be stably incorporated into foods containing high concentrations of ethanol or salts.

JP 2000-212066 A JP 2004-196781 A JP 2008-245588 A JP 2011-050255 A

Health food and beverages today are becoming more diverse in their formulations and contain higher amounts of functional ingredients. Collagen is particularly popular as an ingredient that is effective for improving joint movement and moisturizing the skin, and health drinks containing high concentrations of collagen are now on the market.
However, according to research by the inventors, it has been found that in beverages containing both collagen and coenzyme Q10, when the collagen content is high (for example, 5 g or more of collagen in 50 mL), coenzyme Q10 may separate, precipitate, deposit, or float to the surface, posing stability problems.
The object of the present invention is to provide a water-soluble composition containing coenzyme Q10, which is highly stable and maintains its homogeneity for a long period of time without causing precipitation, deposition, or floating up, even in an aqueous composition containing collagen at a high concentration.

The above problems can be solved by the compositions and methods described below.
(1) A water-soluble composition comprising (A) 1-10% by mass of coenzyme Q10, (B) 1-20% by mass of a polyglycerol fatty acid ester, (C) glycerin, and (D) water, wherein the mass ratio of components (A) to (B) is (A):(B)=1:0.8 to 1:2.4, and the average particle size is 70 nm or less.
(2) The water-soluble composition according to (1), wherein the fatty acid of component (B) is at least one selected from stearic acid and palmitic acid.
(3) The water-soluble composition according to (1) or (2), wherein the component (C) is 60 to 90% by mass and the component (D) is 3.2 to 40% by mass.
(4) The water-soluble composition according to any one of claims 1 to 3, wherein the mass ratio of components (C) and (D) is (C):(D) = 19:1 to 2:1.
(5) A method for producing a water-soluble composition comprising (A) 1 to 10% by mass of coenzyme Q10, (B) 1 to 20% by mass of a polyglycerol fatty acid ester, (C) glycerol, and (D) water, the method comprising the step of dispersing or emulsifying coenzyme Q10, a polyglycerol fatty acid ester, and glycerol in water, wherein the mass ratio of components (A) to (B) is (A):(B)=1:0.8 to 1:2.4, and the water-soluble composition has an average particle size of 70 nm or less.
(6) An aqueous composition comprising collagen, water, and the water-soluble composition according to any one of (1) to (4). (7) The aqueous composition according to (6), having a collagen concentration of 5 to 25% by mass.
(8) A method for producing the aqueous composition according to (6) or (7) above, by adding the water-soluble composition according to (1) to (4) above to an aqueous solution containing collagen.
(9) The method according to (8), wherein the collagen concentration in the aqueous solution is 5 to 25% by mass.
(10) A method for stabilizing coenzyme Q10 by adding the water-soluble composition described in (1) to (4) to an aqueous solution containing collagen.
(11) The method according to (10), wherein the amount of collagen is 5 to 25% by mass when the total amount of the aqueous solution and the water-soluble composition is 100% by mass.

The Coenzyme Q10-containing water-soluble composition of the present invention is usually a liquid emulsion composition, and while it contains fat-soluble Coenzyme Q10, when added to an aqueous liquid, Coenzyme Q10 does not separate, precipitate, deposit or float, even in an aqueous composition containing high concentrations of collagen, and has excellent long-term storage stability, making it possible to provide a variety of health food beverages, such as beverages that contain both collagen and Coenzyme Q10.
In addition, the Coenzyme Q10-containing water-soluble composition of the present invention has the advantage of being highly water-soluble, thereby improving the absorbability of Coenzyme Q10.

The coenzyme Q10-containing water-soluble composition of the present invention comprises (A) 1-10% by mass of coenzyme Q10, (B) 1-20% by mass of polyglycerol fatty acid ester, (C) glycerin, and (D) water, the mass ratio of components (A) and (B) being (A):(B)=1:0.8-1:2.4, and the average particle size is 70 nm or less.

The amounts of each component contained in the coenzyme Q10-containing water-soluble composition of the present invention are described below.

(Coenzyme Q10)
The amount of coenzyme Q10 blended in the coenzyme Q10-containing water-soluble composition of the present invention is 1 to 10% by mass, preferably 2 to 8% by mass, and particularly preferably 3 to 6% by mass.

(Polyglycerol fatty acid ester)
As the polyglycerol fatty acid ester of the coenzyme Q10-containing water-soluble composition of the present invention, esters of polyglycerols of various degrees of polymerization, such as diglycerol, tetraglycerol, hexaglycerol, decaglycerol, etc., or mixtures thereof, and saturated or unsaturated fatty acids of various chain lengths can be used.
Examples of the polyglycerol fatty acid ester used in the coenzyme Q10-containing water-soluble composition of the present invention include polyglycerol stearic acid ester, polyglycerol palmitic acid ester, polyglycerol lauric acid ester, polyglycerol oleic acid ester, polyglycerol myristic acid, polyglycerol behenic acid ester, polyglycerol linoleic acid ester, etc., and these can be used alone or in combination of two or more. Among these, it is preferable to use one or more selected from polyglycerol stearic acid ester and polyglycerol palmitic acid ester.
The content of the polyglycerol fatty acid ester in the coenzyme Q10-containing water-soluble composition of the present invention is 1 to 20% by mass, preferably 2 to 15% by mass, and particularly preferably 3 to 10% by mass.

As the polyglycerol fatty acid ester of the coenzyme Q10-containing water-soluble composition of the present invention, various commercially available products can be appropriately used, such as products manufactured by Nikko Chemicals under the trade names "DECAGLYN1-SVEX" and "DECAGLYN1-PVEX."

(Glycerin)
The amount of glycerin blended in the coenzyme Q10-containing water-soluble composition of the present invention is 60 to 90% by mass, preferably 65 to 90% by mass.

(water)
The content of water in the Coenzyme Q10-containing water-soluble composition of the present invention is 3.2 to 40% by mass, preferably 4.0 to 30% by mass, and particularly preferably 4.5 to 20% by mass.

(Mixing ratio)
Next, the mass ratio of component (A) to component (B) and the mass ratio of component (C) to component (D) in the coenzyme Q10-containing water-soluble composition of the present invention will be described.

In the coenzyme Q10-containing water-soluble composition of the present invention, the ratio of (A):(B) is 1:0.8 to 1:2.4, preferably 1:1 to 1:2. Also, the ratio of (C):(D) is 19:1 to 2:1, preferably 9:1 to 3:1.

The coenzyme Q10-containing water-soluble composition of the present invention is an emulsion composition having an average particle size of 70 nm or less. In order to make the average particle size of the emulsion composition 70 nm or less, it is necessary to stir and homogenize the composition using a homomixer, high-pressure homogenizer, or the like. The suitable rotation speed and stirring time of the homomixer, etc. cannot be generalized because they vary depending on the turbine diameter of the homomixer, etc. and the amount of emulsion to be processed. However, for example, a water-soluble composition having an average particle size of 70 nm or less can be obtained by stirring at 2500 to 14,000 rpm, preferably 3,000 to 12,000 rpm, for 1 minute to 10 hours, preferably 4 minutes to 8 hours. When a composition having the blending components and blending amounts specified in the present invention is stirred for a long time using a homomixer, etc. at a high rotation speed, the average particle size becomes small, but as long as the average particle size is 70 nm or less, the desired effect can be obtained, so there is no need to stir for a longer time than that.

When the coenzyme Q10-containing water-soluble composition of the present invention is added to an aqueous liquid, particularly an aqueous solution containing collagen, the coenzyme Q10 does not separate, precipitate, deposit or float even when mixed with the aqueous solution produced thereby in which collagen is present at a high concentration, so that a health food beverage that simultaneously contains collagen and coenzyme Q10 and has excellent storage stability can be provided.

(collagen)
The collagen that is made to coexist with the water-soluble composition containing coenzyme Q10 of the present invention can be used without any particular limitation as long as it is suitable for oral intake.For example, collagen itself can be used, or collagen in the form of collagen peptide obtained by treatment such as hydrolysis or thermal denaturation can be used, and one or more selected from these can be used.
Although there is no particular limitation on the collagen concentration in the aqueous solution containing collagen to be coexisted with the coenzyme Q10-containing water-soluble composition of the present invention, it is particularly preferable to set the concentration so that an aqueous composition having a collagen concentration of 5 to 25% by mass is generated after adding the coenzyme Q10-containing water-soluble composition. In particular, when using an aqueous solution containing a high collagen concentration, for example, a high concentration of 5 g/50 ml or more or 10 g/50 mL or more of collagen, the effect of using the coenzyme Q10-containing water-soluble composition of the present invention is significantly exhibited.

(Production method)
The Coenzyme Q10-containing aqueous composition of the present invention can be produced by any known method, such as dispersing or emulsifying a fat-soluble component.

For example, coenzyme Q10 is added to glycerin (or polyglycerin fatty acid ester), which is heated to 50°C to 80°C to dissolve the coenzyme Q10, and then water and polyglycerin fatty acid ester (or glycerin) are added and mixed in a water bath of 50°C to 80°C. While maintaining the liquid temperature at 50°C to 70°C, the mixture is stirred and emulsified using a homomixer to obtain a water-soluble composition with an average particle size of 70 nm or less.

The rotation speed and time of the homomixer depend on the amount of emulsion to be processed. For example, for a 0.2 L scale, the rotation speed and time of the homomixer are 4,000 to 12,000 for a TK homomixer MARK II (manufactured by Primix Corporation).
When the mixture is stirred at 500 rpm for 5 minutes or more, a water-soluble composition with an average particle size of 70 nm or less is obtained. It is preferable to quickly cool the emulsion obtained by the homomixer treatment to 40° C. or less.

The water-soluble composition containing coenzyme Q10 of the present invention is dispersed and emulsified until the average particle size is 70 nm or less. By setting the average particle size within the above range, the water-soluble composition containing coenzyme Q10 of the present invention can be uniformly dispersed in an aqueous solution containing collagen.

Next, the present invention will be described in more detail with reference to examples, but the present invention is not limited to the following examples.

(Examples 1 to 6 and Comparative Examples 1 to 5)
In Examples 1 to 6 and Comparative Examples 1 to 5, the change in collagen resistance of the Coenzyme Q10-containing water-soluble composition of the present invention due to the difference in the blending ratio of each component was evaluated.
(Sample Preparation)
According to the blending ratio in Table 1 below, polyglycerol fatty acid ester (decaglycerol monostearate: DECAGLYN1-SVEX (manufactured by Nikko Chemicals)) and coenzyme Q10 were placed in a beaker and mixed in a water bath at 60°C.
Next, glycerin and water were added, and the mixture was gently stirred in a water bath at 60°C. While maintaining the temperature at 60°C, the mixture was emulsified by stirring at 8,000 rpm for 15 minutes using a TK Homomixer MARK II (turbine diameter 28 mm, manufactured by Primix Corporation). The emulsion was then cooled to room temperature on ice, and the particle size was measured.

(Stability evaluation in aqueous solutions containing collagen)
Collagen was dissolved in water to a final concentration of 10 g/50 mL, and the pH was adjusted to 4.0 with citric acid. The above-prepared sample (emulsion) was added and mixed to a coenzyme Q10 concentration of 30 mg/50 mL, and then filtered through filter paper (No. 6, Advantec). The filtrate was sterilized by heating in a 95°C hot bath for 20 minutes, cooled, and stored in a thermostatic chamber at 40°C and 75% relative humidity, and the appearance was observed over time.

(Evaluation Method)
The appearance after storage for 1 day, 14 days, 30 days, and 60 days was visually evaluated according to the following evaluation criteria.
◎: No change from immediately after preparation ○: Slight haze or turbidity is observed △: Suspended matter is observed ×: Sedimentation, separation, or deposition is observed

(Method for measuring average particle size)
The sample (emulsion) prepared above at room temperature was diluted 100 times with water, and the particle size was measured using a dynamic light scattering particle size distribution analyzer (Zetasizer Pro: manufactured by Malvern Instruments). The Z-average value was was taken as the average particle size (nm).

(result)

(Examples 7 to 9 and Comparative Examples 6 to 9)
In Examples 7 to 9 and Comparative Examples 6 to 9, changes in collagen resistance of the Coenzyme Q10-containing water-soluble composition of the present invention due to differences in particle size were evaluated.

(Sample Preparation)
According to the blending ratio in Table 2 below, polyglycerol fatty acid ester (decaglycerol monostearate: DECAGLYN1-SVEX (manufactured by Nikko Chemicals)) and coenzyme Q10 were placed in a beaker and mixed in a water bath at 60°C.
Next, glycerin and water were added, and the mixture was stirred gently in a water bath at 60° C., and emulsified by stirring at 8,000 rpm using a TK homomixer MARK II (manufactured by Primix Corporation), and samples were appropriately taken during the stirring process.
The sampled emulsion was cooled to room temperature on ice, and the particle size was measured.

The stability in an aqueous solution containing collagen was evaluated in the same manner as in Examples 1 to 6.

(result)

(Examples 10 to 11)
In Examples 10 and 11, the change in collagen resistance depending on the type of polyglycerol fatty acid ester was evaluated.

(Sample Preparation)
According to the blending ratio in Table 3 below, glycerin and coenzyme Q10 were placed in a beaker and dissolved in a water bath at 60° C. Next, polyglycerin fatty acid ester (decaglycerin monopalmitate: DECAGLYN1-PVEX (manufactured by Nikko Chemicals), or decaglycerin monostearate: DECAGLYN1-SVEX (manufactured by Nikko Chemicals)) and water were added and gently stirred in a water bath at 60° C., and emulsified by stirring at 8000 rpm for 60 minutes at 60° C. using a TK homomixer MARKII (manufactured by Primix Corporation).
The sampled emulsion was cooled to room temperature on ice, and the particle size was measured.

The stability in an aqueous solution containing collagen was evaluated in the same manner as in Examples 1 to 6.

(result)

Claims (10)

A water-soluble composition comprising (A) 1-10% by mass of coenzyme Q10, (B) 1-20% by mass of a polyglycerol fatty acid ester, (C) 60-90% by mass of glycerol, and (D) 4.0-30% by mass of water, wherein the mass ratio of components (A) to (B) is (A):(B)=1:0.8-1:2.4, and the average particle size is 70 nm or less. The water-soluble composition according to claim 1, wherein the fatty acid of component (B) is at least one selected from stearic acid and palmitic acid. 3. The water-soluble composition according to claim 1 , wherein the mass ratio of components (C) and (D) is (C):(D)=19:1 to 2:1. A method for producing a water-soluble composition comprising (A) 1-10% by mass of coenzyme Q10, (B) 1-20% by mass of a polyglycerol fatty acid ester, (C) 60-90% by mass of glycerol, and (D) 4.0-30% by mass of water, wherein the mass ratio of components (A) to (B) is (A):(B)=1:0.8-1:2.4, the method comprising the step of dispersing or emulsifying coenzyme Q10, a polyglycerol fatty acid ester, and glycerol in water. An aqueous composition comprising collagen, water and the water-soluble composition according to any one of claims 1 to 3 . 6. The aqueous composition according to claim 5, wherein the collagen concentration is 5 to 25% by mass. A method for producing the aqueous composition according to claim 5 or 6 , which comprises adding the water-soluble composition according to any one of claims 1 to 3 to an aqueous solution containing collagen. The method according to claim 7 , wherein the collagen concentration in the aqueous composition is 5 to 25% by mass. A method for stabilizing coenzyme Q10 by adding the water-soluble composition according to any one of claims 1 to 3 to an aqueous solution containing collagen. The method according to claim 9 , wherein the amount of collagen is 5 to 25% by mass when the total amount of the aqueous solution and the water-soluble composition is taken as 100% by mass.