A tea polyphenol blend, its preparation method and application
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- HANGZHOU QIANDAOHU TIANXIN CO LTD
- Filing Date
- 2026-04-07
- Publication Date
- 2026-07-21
AI Technical Summary
Tea polyphenols are prone to oxidation and polymerization in cosmetics, resulting in discoloration and degradation of active ingredients, leading to extremely low addition levels and limited widespread application.
By preparing tea polyphenol blends, protein-silk peptide powder and pullulan polysaccharide are used to form non-covalent bonds with tea polyphenols, forming a tight network structure that prevents the oxidation of tea polyphenols and locks them in the network, while hydrogen bonding enhances stability.
This technology enables the addition and stability of tea polyphenols in cosmetics, avoiding oxidation, discoloration, and degradation of active ingredients, thereby improving the shelf-life stability and skin efficacy of cosmetics.
Smart Images
Figure CN121987544B_ABST
Abstract
Description
Technical Field
[0001] This invention relates to a blend, its preparation method, and its application, particularly a tea polyphenol blend, its preparation method, and its application. Background Technology
[0002] Tea polyphenols, also known as tea tannins or tea tannins, are a general term for a class of polyhydroxyphenolic compounds contained in tea. The components include catechins (flavanols), flavonoids, flavonols, anthocyanins, phenolic acids, condensed phenolic acids, and polymeric phenols. Among them, catechins are the main components of tea polyphenols, including catechin (C), epicatechin (EC), epicatechin gallatechin (ECG), etc.
[0003] The oxidative polymerization of tea polyphenols is mainly determined by both enzymatic and non-enzymatic factors. Tea polyphenol oxidase is a secondary metabolite found in tea trees, but it is often depleted during the high-temperature drying and powdering process of tea polyphenol extraction. Therefore, in cosmetic applications, the oxidative browning of tea polyphenols is often due to non-enzymatic oxidative polymerization, which causes the polyphenols to polymerize into polymers. Furthermore, the polymerization process leads to the degradation of active ingredients, and the polymerization reaction is irreversible. Studies have shown that tea polyphenols have poor thermal stability, with their content gradually decreasing as temperature increases. This means that although tea polyphenols possess strong biological activity, their unstable structure makes them highly susceptible to oxidative polymerization, resulting in discoloration and degradation of active ingredients. Consequently, tea polyphenols cannot be widely used in the cosmetics or food industries, and their addition in cosmetics is often extremely low, frequently within trace amounts. Moreover, it is difficult to guarantee the shelf stability and effectiveness of cosmetics containing tea polyphenols. Summary of the Invention
[0004] The purpose of this invention is to provide a tea polyphenol blend, its preparation method, and its application. It overcomes the problems of oxidative polymerization of tea polyphenols leading to discoloration and degradation of active ingredients in existing technologies. This solves the problem that tea polyphenols are often added in extremely low amounts in cosmetics, limiting their widespread application and improving their performance in cosmetic applications.
[0005] The technical solution of the present invention is: a tea polyphenol blend, comprising, by weight, 0.2-3 parts tea polyphenols, 0.5-5 parts protein-silk peptide powder and 0.2-5 parts pullulan.
[0006] In the aforementioned tea polyphenol blend, the protein-silk fibroin peptide powder is obtained by uniformly mixing silk fibroin protein and soluble silk fibroin peptide powder in a weight ratio of 7:3.
[0007] A method for preparing a tea polyphenol blend includes the following steps:
[0008] S1. The degummed silk is purified to obtain silk fibroin powder. After hydrolysis of the silk fibroin, soluble silk fibroin peptide powder with a molecular weight of 450-2000 is obtained, with the sequence Ala-Ser-Gly-Ser-Ala.
[0009] S2. Mix silk fibroin and soluble silk peptide powder in a weight ratio of 7:3 until uniform and set aside to obtain protein-silk peptide powder.
[0010] S3. Dissolve pullulan in water to prepare a 20% solution and refrigerate at 4°C for later use.
[0011] S4. Mix protein-silk peptide powder and glycerin in a weight ratio of 1:5, and stir at 50-70 rpm at 20-30℃ until homogeneous to form product A with uniformity.
[0012] S5. Slowly add tea polyphenols to product A and stir at 50-70 rpm at 20-30℃ until the mixture is uniform to obtain product B. The weight ratio of tea polyphenols to protein-silk peptide powder in product A is 1:2.
[0013] S6. Adjust the pH of product B to 3.5-4.0 with citric acid, and slowly add pullulan polysaccharide solution to product B while stirring until completely mixed to obtain product C. The dry weight ratio of pullulan polysaccharide and protein-silk fibroin peptide powder in product B is 1:1.
[0014] S7. After placing the obtained product C at 4℃ for 24 hours, place it in a centrifuge tube and centrifuge at 10000rpm for 10 minutes. Remove the top and bottom clear liquids and collect the remaining liquid in the centrifuge tube to obtain product D.
[0015] S8. Place product D in an ultrasonic instrument, adjust the output power to 20kHz and the working time to 10s, and treat it in an ice bath for 10 minutes every 2s to obtain the finished tea polyphenol blend.
[0016] The application of a tea polyphenol blend as an active ingredient in the cosmetics industry.
[0017] The aforementioned application of a tea polyphenol blend as an active ingredient in the cosmetics field includes cosmetic types such as serums, lotions, and creams.
[0018] The aforementioned application of a tea polyphenol blend as an active ingredient in the cosmetics field refers to a cosmetic that is a W / O / W type emulsion multi-emulsion.
[0019] In the aforementioned application of a tea polyphenol blend as an active ingredient in the cosmetics field, the cosmetics include a first aqueous phase, an oil phase, and a second aqueous phase.
[0020] In the aforementioned application of a tea polyphenol blend as an active ingredient in the cosmetics field, the first aqueous phase, by weight, comprises 10 parts of the tea polyphenol blend and 10 parts of deionized water.
[0021] In the application of the aforementioned tea polyphenol blend as an active ingredient in the cosmetics field, the second aqueous phase, by weight, comprises 50 parts water, 1 part phenoxyethanol, 0.5 parts 1,2-hexanediol, 2 parts PEG-100 stearate, 0.1 parts daily fragrance, 10 parts glycerin, and 0.5 parts carbomer.
[0022] In the application of the aforementioned tea polyphenol blend as an active ingredient in the cosmetics field, the oil phase, by weight, includes 10 parts squalane, 5 parts cetearyl alcohol, 5 parts caprylic / capric triglyceride, 0.5 parts tocopherol, and 2 parts glyceryl stearate.
[0023] Compared with the prior art, the present invention has the following advantages:
[0024] This application utilizes a non-covalent bonding mechanism between protein-silk fibroin peptide powder and tea polyphenols to form a blend. The entanglement of pullulan polysaccharide within the system further strengthens the bond of the blend. Under certain conditions, protein-silk fibroin peptide powder and tea polyphenols can combine, with the polysaccharide forming a network structure that locks the tea polyphenols within the network, effectively preventing polymerization between tea polyphenols. Simultaneously, tea polyphenols, acting as hydrogen bond donors, enhance the interaction between the polysaccharide and the modified silk peptides. These three elements mutually restrain and constrain each other, resulting in a more stable self-assembled system. The formed network structure further delays the browning of tea polyphenols, making them more stable and less prone to oxidation. This allows for the addition of high-content tea polyphenols in cosmetics without browning, and the product exhibits virtually no discoloration in accelerated testing. Furthermore, this invention can suppress the degradation risk of functional components (such as catechins) in tea polyphenols due to structural instability, avoid the problem of efficacy loss of tea polyphenols due to degradation of active ingredients, and achieve high retention of active ingredients in tea polyphenols. When tea polyphenol blends are applied to cosmetics, the multi-emulsification system "protects" tea polyphenols in the innermost layer, effectively slowing down the oxidation of tea polyphenols, ensuring their shelf life stability, and can more effectively reduce the content of melanin in the skin and improve skin tone. Attached Figure Description
[0025] Figure 1 These are the infrared spectra of Example 1 and Comparative Group 1;
[0026] Figure 2These are microscopic images of Example 2 and Comparative Group 2;
[0027] Figure 3 This is a graph showing the accelerated stability test results of Example 2; Figure 4 This is a graph showing the accelerated stability test results for control group 2. Detailed Implementation
[0028] The present invention will be further described below with reference to the accompanying drawings and embodiments, but this should not be construed as limiting the present invention.
[0029] Example 1. A tea polyphenol blend comprising 0.2-3 parts tea polyphenols, 0.5-5 parts protein-silk fibroin peptide powder and 0.2-5 parts pullulan, wherein the protein-silk fibroin peptide powder is obtained by uniformly mixing silk fibroin protein and soluble silk fibroin peptide powder in a weight ratio of 7:3.
[0030] A method for preparing a tea polyphenol blend includes the following steps:
[0031] S1. The degummed silk is purified to obtain silk fibroin powder. After hydrolysis of the silk fibroin, soluble silk fibroin peptide powder with a molecular weight of 450-2000 is obtained, with the sequence Ala-Ser-Gly-Ser-Ala.
[0032] S2, silk fibroin and soluble silk peptide powder are mixed evenly in a weight ratio of 7:3 to obtain protein-silk peptide powder.
[0033] S3. Dissolve pullulan in water to prepare a 20% solution and refrigerate at 4°C for later use.
[0034] S4. Mix protein-silk peptide powder and glycerin in a weight ratio of 1:5, and stir at 50-70 rpm at 20-30℃ until homogeneous to form product A with uniformity.
[0035] S5. Slowly add tea polyphenols to product A and stir at 50-70 rpm at 20-30℃ until the mixture is uniform to obtain product B. The weight ratio of tea polyphenols to protein-silk peptide powder in product A is 1:2.
[0036] S6. Adjust the pH of product B to 3.5-4.0 with citric acid, and slowly add pullulan polysaccharide solution to product B while stirring until completely mixed to obtain product C. The dry weight ratio of pullulan polysaccharide and protein-silk fibroin peptide powder in product B is 1:1.
[0037] S7. After placing the obtained product C at 4℃ for 24 hours, place it in a centrifuge tube and centrifuge at 10000rpm for 10 minutes. Remove the top and bottom clear liquids and collect the remaining liquid in the centrifuge tube to obtain product D.
[0038] S8. Place product D in an ultrasonic instrument, adjust the output power to 20kHz and the working time to 10s, and treat it in an ice bath for 10 minutes every 2s to obtain the finished tea polyphenol blend.
[0039] Example 2. Application of a tea polyphenol blend as an active ingredient in the cosmetics field. The cosmetic types include serums, lotions, and creams.
[0040] The face cream comprises a first aqueous phase, an oil phase, and a second aqueous phase.
[0041] The first aqueous phase, by weight, comprises 10 parts of tea polyphenol blend and 10 parts of deionized water. The preparation process of the first aqueous phase is to mix the obtained tea polyphenol blend with deionized water to obtain the first aqueous phase.
[0042] The second aqueous phase, by weight, comprises 50 parts water, 1 part phenoxyethanol, 0.5 parts 1,2-hexanediol, 2 parts PEG-100 stearate, 0.1 parts fragrance, 10 parts glycerin, and 0.5 parts carbomer. The preparation process of the second aqueous phase involves heating water, phenoxyethanol, 1,2-hexanediol, fragrance, glycerin, carbomer, and PEG-100 stearate to approximately 70°C to dissolve and mix them evenly, thereby obtaining the second aqueous phase.
[0043] The oil phase, by weight, comprises 10 parts squalane, 5 parts cetearyl alcohol, 5 parts caprylic / capric triglyceride, 0.5 parts tocopherol, and 2 parts glyceryl stearate. The preparation process of the oil phase involves heating squalane, cetearyl alcohol, caprylic / capric triglyceride, tocopherol, and glyceryl stearate to about 70°C to dissolve and mix them evenly to obtain the oil phase.
[0044] The preparation process of the face cream is as follows: the first aqueous phase is slowly added dropwise to the oil phase, maintaining a homogenization speed of 5000 rpm. After 5 minutes, the mixture is homogenized to form a W / O emulsion. The W / O emulsion obtained from the first aqueous phase and the oil phase is heated to 70°C. The W / O emulsion is then slowly added to the second aqueous phase, maintaining a homogenization speed of 6000 rpm. After 10 minutes, the mixture is homogenized to form a W / O / W emulsion multi-emulsion, resulting in a face cream containing tea polyphenols.
[0045] Through a series of experimental tests, this application confirms that the tea polyphenol blend has good stability and can slow down the degradation of the effective components of tea polyphenols.
[0046] Unless otherwise specified, the experimental methods used in the following examples are conventional methods; the materials and reagents used are commercially available unless otherwise specified. Comparative group 1 used a tea polyphenol gel containing tea polyphenols, silk fibroin powder, and pullulan, while Example 1 used the tea polyphenol blend described in the examples of this application.
[0047] I. Infrared Spectroscopy Test Experiment.
[0048] Infrared spectroscopy tests were performed on Example 1 and Comparative Group 1, and the test results are shown in the attached figures of the specification. Figure 1 As shown in the figure, 1 represents Example 1, 2 represents Control Group 1, and Wavenumber represents the wave number in cm. -1 Transmittance (%) represents light transmittance, expressed as a percentage (%). As can be seen from the graph, due to the identical substrate, the FTIR curves exhibit essentially the same trend. This is because both contain pullulan and silk fibroin powder, and the curves are located at 3269 cm⁻¹. -1 The absorption peak at the OH group is relatively flat, indicating that the addition of pullulan interacts with tea polyphenols and silk fibroin powder to form hydrogen bonds, reducing the vibration of free OH bonds in the tea polyphenol-silk fibroin-pullulan polyphenol group. However, there is a difference in the infrared spectra between Example 1 and Comparative Group 1, with different key characteristic peaks for C=O and C=C bonds. This is a result of the combined influence of tea polyphenols and soluble silk fibroin peptide powder. In Example 1 and Comparative Group 1, the infrared absorption peak of the C=C double bond changes from 1604 cm⁻¹. -1 Moved to 1620cm -1 This is because, under the conditions of the coexistence of silk fibroin powder, soluble silk fibroin peptide powder, and tea polyphenols, the macromolecular structure of tea polyphenols affects the distribution of the electron cloud, causing an increase in vibrational frequency and resulting in a blue shift of the C=C bond. In addition, the addition of soluble silk fibroin peptide powder also affects the spatial structure of the tea polyphenol-silk fibroin powder, leading to an increase in the "movement" energy of the C=C bond. The combined effect of these two factors increases the vibrational frequency towards higher wavenumbers, resulting in a "blue shift" in infrared absorption. This indicates that, compared to control group 1 without soluble silk fibroin peptide powder, in Example 1, the addition of soluble silk fibroin peptide powder causes the phenolic hydroxyl groups in tea polyphenols to bond with the amino and carboxyl groups in soluble silk fibroin peptide powder via hydrogen bonds. This makes the intermolecular forces between tea polyphenols, silk fibroin, and silk fibroin peptides stronger and tighter, thereby enhancing and stabilizing the network structure of silk fibroin, silk fibroin peptides, and tea polyphenols, and improving the thermal stability of the sample.
[0049] II. Accelerated Experimentation.
[0050] Accelerated testing was conducted on Example 1 and Control Group 1 at temperatures of 25°C and 45°C, and humidity of 75% ± 5% RH, respectively, to simulate the product's performance during its shelf life. Samples were taken on days 0 and 7 of the 45°C test to test the changes in the content of tea polyphenols and catechins, thereby determining the degradation of the effective components in tea polyphenols. The results are shown in Table 1.
[0051] Table 1. Change rate of active ingredient content in tea polyphenols after 7 days of accelerated testing at 45℃
[0052]
[0053] As shown in Table 1, the contents of the active ingredients EGCG, EGC, EC, ECG, and C in tea polyphenols in Example 1 did not change significantly after 7 days of accelerated testing. However, the contents of these active ingredients in control group 1 were significantly reduced. This indicates that polymerization of tea polyphenols occurred during the accelerated testing, leading to degradation of the effective components in the test samples and consequently, a change in their appearance. The tea polyphenol blend of this invention can effectively slow down the degradation of the active ingredients in tea polyphenols.
[0054] Samples were taken on days 0 and 7 of accelerated experiments at 25℃ and 45℃ to test their antioxidant function, thereby determining the effectiveness of the components in tea polyphenols. The results are shown in Table 2.
[0055] DPPH free radical scavenging rate test method: Dissolve DPPH powder in anhydrous ethanol and dilute to a 2 mmol / L stock solution; take 2 mL of diluted sample (diluted 200 times with 95% ethanol) and add 2 mL of DPPH working solution diluted to 0.2 mmol / L. After vortexing, react at room temperature in the dark for 30 min, and measure the absorbance value Ai at 517 nm; use anhydrous ethanol as a blank to zero the sample, and use 2 mL of the corresponding concentration of test sample solution plus 2 mL of anhydrous ethanol as a control (Aj); the absorbance value Ac is obtained by adding 2 mL of 95% ethanol to 2 mL of DPPH working solution; then the scavenging ability of the test sample for DPPH free radicals is: .
[0056] Table 2: DPPH free radical scavenging rate test results
[0057]
[0058] Samples from Example 1 and Control Group 1, which underwent accelerated testing at 25°C and 45°C, were taken on days 0 and 7 to test their antioxidant function, thereby determining the effectiveness of the active ingredients in tea polyphenols. As can be seen from the table above, the tea polyphenol blend of the present invention has a very good protective effect on the active ingredients and efficacy of tea polyphenols.
[0059] III. Testing of cosmetic applications containing tea polyphenols.
[0060] Example 2 is a multi-emulsification system face cream containing tea polyphenol blends and prepared according to the process described in the example.
[0061] Group 2 consists of face creams containing the same amount of tea polyphenols obtained through different preparation processes from tea polyphenol gel containing tea polyphenols, protein-silk peptide powder, and pullulan.
[0062] Microscopic particle size analysis was performed on Example 2 and Comparative Group 2. The particle size distribution showed that a multi-component cosmetic cream containing tea polyphenol blends was successfully prepared according to the process described in the embodiments of this application.
[0063] Accelerated experiments were conducted on Example 2 and Comparative Group 2, placing them at -10℃, 5℃, 25℃, 40℃, and 45℃ for 90 days. The experimental results are as per the instruction manual. Figure 3-4 As shown, in control group 2, significant browning was observed in the face cream after 90 days under accelerated 45°C testing. This was due to the polymerization of active ingredients in the tea polyphenols, leading to the transformation of tea polyphenols into polymers. In Example 2, the face cream appearance remained essentially unchanged after 90 days under accelerated testing compared to other test conditions. This indicates that the face cream prepared using multiple emulsions can effectively isolate the browning problem of tea polyphenols caused by external factors, thereby effectively delaying the application stability of tea polyphenols.
[0064] Safety testing of the face cream involved skin patch tests on Example 2 and Control Group 2. The results are shown in the table below:
[0065] Table 3: Safety Test Results of Face Cream
[0066]
[0067] As can be seen from Table 3, the tea polyphenol face cream prepared using the formula of the present invention passed the human patch safety test, and no adverse reactions were observed in any of the participants. This indicates that the face cream prepared by the method of the present invention is safe and can be widely used in cosmetics.
[0068] The efficacy of the face creams prepared in Example 2 and Control Group 2 was tested using an ultraviolet-induced human skin melanization model to assess their skin brightening effect. The test results are as follows:
[0069] Table 4: Results of Face Cream Efficacy Test
[0070]
[0071] Note: P<0.05 indicates a significant difference, and P<0.001 indicates an extremely significant difference.
[0072] As can be seen from Table 4, the tea polyphenol face cream prepared using the formula of the present invention is significantly better than the control group 2 in terms of efficacy. It can more effectively reduce melanin content and improve skin tone. This shows that the face cream of the present invention can effectively protect the activity of tea polyphenols so that they can better exert their effects on the skin and avoid affecting their biological activity before they have exerted their effects.
Claims
1. A blend of tea polyphenols, characterized in that, The mixture comprises, by weight, 0.2-3 parts tea polyphenols, 0.5-5 parts protein-silk peptide powder, and 0.2-5 parts pullulan, and the preparation method of the tea polyphenol blend includes the following steps: S1. The degummed silk is purified to obtain silk fibroin powder. After hydrolysis of the silk fibroin, soluble silk fibroin peptide powder with a molecular weight of 450-2000 is obtained, with the sequence Ala-Ser-Gly-Ser-Ala. S2. Mix silk fibroin and soluble silk peptide powder in a weight ratio of 7:3 until uniform and set aside to obtain protein-silk peptide powder. S3. Dissolve pullulan in water to prepare a 20% solution and refrigerate at 4°C for later use. S4. Mix protein-silk peptide powder and glycerin in a weight ratio of 1:5, and stir at 50-70 rpm at 20-30℃ until homogeneous to form product A with uniformity. S5. Slowly add tea polyphenols to product A and stir at 50-70 rpm at 20-30℃ until the mixture is uniform to obtain product B. The weight ratio of tea polyphenols to protein-silk peptide powder in product A is 1:
2. S6. Adjust the pH of product B to 3.5-4.0 with citric acid, and slowly add pullulan polysaccharide solution to product B while stirring until completely mixed to obtain product C. The dry weight ratio of pullulan polysaccharide and protein-silk fibroin peptide powder in product B is 1:
1. S7. After placing the obtained product C at 4℃ for 24 hours, place it in a centrifuge tube and centrifuge at 10000rpm for 10 minutes. Remove the top and bottom clear liquids and collect the remaining liquid in the centrifuge tube to obtain product D. S8. Place product D in an ultrasonic instrument, adjust the output power to 20kHz and the working time to 10s, and treat it in an ice bath for 10 minutes every 2s to obtain the finished tea polyphenol blend.
2. The application of the tea polyphenol blend according to claim 1 as an active ingredient in the preparation of cosmetics with whitening effects.
3. The application according to claim 2, characterized in that: The cosmetic types mentioned include serums, lotions, and creams.
4. The application according to claim 3, characterized in that: The cosmetic product in question is a W / O / W type emulsion multi-emulsion.
5. The application according to claim 3, characterized in that: The cosmetic product comprises a first aqueous phase, an oil phase, and a second aqueous phase.
6. The application according to claim 5, characterized in that: The first aqueous phase, by weight, comprises 10 parts of tea polyphenol blend and 10 parts of deionized water.
7. The application according to claim 5, characterized in that: The second aqueous phase, by weight, comprises 50 parts water, 1 part phenoxyethanol, 0.5 parts 1,2-hexanediol, 2 parts PEG-100 stearate, 0.1 parts daily fragrance, 10 parts glycerin, and 0.5 parts carbomer.
8. The application according to claim 5, characterized in that: The oil phase, by weight, comprises 10 parts squalane, 5 parts cetearyl alcohol, 5 parts caprylic / capric triglyceride, 0.5 parts tocopherol, and 2 parts glyceryl stearate.