CN115212151A - Extraction method of gentian extract, gentian extract and application of gentian extract - Google Patents
Extraction method of gentian extract, gentian extract and application of gentian extract Download PDFInfo
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- CN115212151A CN115212151A CN202210929702.2A CN202210929702A CN115212151A CN 115212151 A CN115212151 A CN 115212151A CN 202210929702 A CN202210929702 A CN 202210929702A CN 115212151 A CN115212151 A CN 115212151A
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K8/00—Cosmetics or similar toiletry preparations
- A61K8/18—Cosmetics or similar toiletry preparations characterised by the composition
- A61K8/96—Cosmetics or similar toiletry preparations characterised by the composition containing materials, or derivatives thereof of undetermined constitution
- A61K8/97—Cosmetics or similar toiletry preparations characterised by the composition containing materials, or derivatives thereof of undetermined constitution from algae, fungi, lichens or plants; from derivatives thereof
- A61K8/9783—Angiosperms [Magnoliophyta]
- A61K8/9789—Magnoliopsida [dicotyledons]
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61P—SPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
- A61P17/00—Drugs for dermatological disorders
- A61P17/04—Antipruritics
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61P—SPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
- A61P29/00—Non-central analgesic, antipyretic or antiinflammatory agents, e.g. antirheumatic agents; Non-steroidal antiinflammatory drugs [NSAID]
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61Q—SPECIFIC USE OF COSMETICS OR SIMILAR TOILETRY PREPARATIONS
- A61Q19/00—Preparations for care of the skin
- A61Q19/005—Preparations for sensitive skin
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K2800/00—Properties of cosmetic compositions or active ingredients thereof or formulation aids used therein and process related aspects
- A61K2800/80—Process related aspects concerning the preparation of the cosmetic composition or the storage or application thereof
- A61K2800/805—Corresponding aspects not provided for by any of codes A61K2800/81 - A61K2800/95
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K2800/00—Properties of cosmetic compositions or active ingredients thereof or formulation aids used therein and process related aspects
- A61K2800/80—Process related aspects concerning the preparation of the cosmetic composition or the storage or application thereof
- A61K2800/82—Preparation or application process involves sonication or ultrasonication
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Abstract
The invention discloses an extraction method of a gentian extract, the gentian extract and application thereof. The extraction method comprises the following steps: providing gentian and a eutectic solvent, wherein the gentian is the whole gentiana rigescens; pretreating the whole gentiana rigescens to obtain gentiana rigescens powder; mixing the gentiana rigescens powder with a eutectic solvent, carrying out ultrasonic treatment, centrifuging to remove impurities, and concentrating to obtain the gentiana rigescens extract. The ultrasonic-assisted deep eutectic solvent extraction method is a green extraction separation method, improves the extraction efficiency, shortens the extraction time, reduces the use of organic solvents, and is green and environment-friendly. In addition, the invention extracts the whole gentiana rigescens, can increase the utilization rate of gentiana rigescens resources, reduces the waste treatment of the root leaves of gentiana rigescens, and achieves the effect of changing waste into valuables. The gentian extract disclosed by the invention has the effects of resisting inflammation, relieving itching, repairing and the like, and can be directly applied to the field of cosmetics.
Description
Technical Field
The invention relates to the technical field of plant extraction, and particularly relates to an extraction method of a gentian extract, the gentian extract and application of the gentian extract.
Background
Gentiana scabra Bunge (Gentiana scabra Bunge) is a perennial herb of Gentianaceae, mainly produced in northeast and Yunnan, and is considered by traditional Chinese medicine to be bitter and cold in nature and taste; it enters liver and gallbladder meridians; has effects in clearing away heat, eliminating dampness, purging liver-fire and gallbladder-fire, and invigorating stomach. The Gentiana rigescens, which is also called as "Gentiana rigescens", "Sophora alopecuroides", "herring gall", "Gentiana microphylla", and the like, is a perennial herb of Gentianaceae, mainly produced in Yunnan province, is one of the traditional Chinese medicine Gentiana scabra varieties and is recorded as a folk important medicine. Because it has the effects of clearing away damp-heat, benefiting liver and gallbladder, invigorating stomach, sterilizing, resisting inflammation, reducing weight, etc., it is used as bitter stomachic in modern medicine.
At present, the methods adopted for extracting the gentian extract are a cold soaking method, a warm extraction method, a cold soaking grinding method, a Soxhlet extraction method, a water and alcohol extraction method and the like, and the traditional extraction methods all use an organic solvent as an extraction solvent, so that the solvent consumption is large and the process is long in time consumption.
Accordingly, the prior art is yet to be improved and developed.
Disclosure of Invention
In view of the defects of the prior art, the invention aims to provide an extraction method of a gentian extract, the gentian extract and application thereof, and aims to solve the problems that the existing extraction method takes an organic solvent as an extraction solvent, the solvent consumption is large, the process is time-consuming, and the utilization rate of gentian raw materials is low.
The technical scheme of the invention is as follows:
in a first aspect of the present invention, there is provided a method for extracting a gentian extract, comprising the steps of:
providing gentiana and a eutectic solvent, wherein the gentiana is a whole gentiana rigescens;
pretreating the whole gentiana rigescens to obtain gentiana rigescens powder;
mixing the gentiana rigescens powder with a eutectic solvent, carrying out ultrasonic treatment, centrifuging to remove impurities, and concentrating to obtain the gentiana rigescens extract.
Optionally, the step of pretreating the whole gentiana rigescens specifically comprises: cleaning whole Gentiana rigescens with water, air drying, drying at 40-60 deg.C for more than 10 hr, pulverizing, and sieving with 40-80 mesh pharmacopoeia sieve.
Optionally, the method for preparing the eutectic solvent comprises the following steps: and mixing the hydrogen bond acceptor and the hydrogen bond donor according to a preset molar ratio, and heating for a preset time under the conditions of a preset temperature and a preset rotating speed to obtain the eutectic solvent.
Optionally, the hydrogen bond acceptor is betaine, and the hydrogen bond donor is one or two of 1,3-butanediol, urea, glycerol, 1,3-propanediol and lactic acid;
and/or the molar ratio of the hydrogen bond acceptor to the hydrogen bond donor is 1:2-1.
Optionally, the preset temperature is 60-90 ℃, the preset time is 30min-2h, and the preset rotating speed is 400-800rpm.
Optionally, the mass-to-volume ratio of the gentiana rigescens powder to the eutectic solvent is 1:20-50.
Optionally, the ultrasonic treatment time is 10-30min, the ultrasonic treatment temperature is 40-60 ℃, and the ultrasonic power is 200-500W.
Optionally, the step of removing impurities by centrifugation and concentrating specifically includes: centrifuging at 2000-3000rpm to obtain supernatant and residue, extracting the residue with the eutectic solvent for 1-3 times, collecting supernatant, and concentrating.
In a second aspect of the present invention, a gentian extract is provided, wherein the gentian extract is obtained by extraction using the extraction method of the gentian extract of the present invention.
In a third aspect of the present invention, there is provided a use of the gentian extract according to the present invention for preparing a cosmetic having a sensitive skin repairing effect.
Has the advantages that: the extraction method of the gentiana rigescens extract adopts an ultrasonic-assisted extraction technology, utilizes ultrasonic cavitation to destroy plant cell walls, and is beneficial to dissolving and diffusing substances in cells; and the eutectic solvent which has the advantages of no toxicity, biodegradability, recoverability and easy preparation is used as the extractant. Compared with the traditional extraction method, the ultrasonic-assisted eutectic solvent extraction method is a green extraction separation method, improves the extraction efficiency, shortens the extraction time, reduces the use of organic solvents, and is green and environment-friendly. In addition, the invention extracts the whole gentiana rigescens, can increase the utilization rate of gentiana rigescens resources, reduces the waste treatment of the root leaves of gentiana rigescens, and achieves the effect of changing waste into valuables. The gentian extract obtained by the invention has the effects of resisting inflammation, relieving itching, repairing and the like, and can be directly applied to the field of cosmetics.
Drawings
FIG. 1 is a graph based on the results of macrophage cytotoxicity assays for example 3.
Figure 2 is based on the results of keratinocyte cytotoxicity assays for example 3.
FIG. 3 is a graph showing the effect of TNF-. Alpha.inflammatory factor inhibition performed in example 3.
FIG. 4 is a graph showing the effect of inhibiting IL-6 inflammatory factor in example 3.
Detailed Description
The present invention provides a method for extracting a gentian extract, a gentian extract and an application thereof, and the present invention is further described in detail below in order to make the purposes, technical schemes and effects of the present invention clearer and clearer. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
At present, the methods adopted for extracting the gentian extract are a cold soaking method, a warm extraction method, a cold soaking grinding method, a Soxhlet extraction method, a water and alcohol extraction method and the like, and the traditional extraction methods all use an organic solvent as an extraction solvent, so that the solvent consumption is large, and the process is long in time consumption.
Therefore, it is important to find an economical, efficient and green extraction solvent. The eutectic solvent is a two-component or three-component eutectic mixture which is formed by combining a hydrogen bond acceptor and a hydrogen bond donor according to a certain stoichiometric ratio, and the freezing point of the eutectic mixture is obviously lower than the melting point of pure substances of each component. It has the advantages of difficult volatilization, high thermal stability, nontoxicity, biodegradability, easy preparation, low cost and the like, thereby being a novel green solvent.
The inventor finds that the gentian extract is extracted by using the eutectic solvent and combining an ultrasonic technology, and a good effect can be obtained.
Based on this, the embodiment of the present invention provides an extraction method of a gentian extract, which includes the steps of:
providing gentian and a eutectic solvent, wherein the gentian is the whole gentiana rigescens;
pretreating the whole gentiana rigescens to obtain gentiana rigescens powder;
mixing the gentiana rigescens powder with a eutectic solvent, carrying out ultrasonic treatment, centrifuging to remove impurities, and concentrating to obtain the gentiana rigescens extract.
According to the method for extracting the gentiana rigescens extract, an ultrasonic-assisted extraction technology is adopted, and ultrasonic cavitation is utilized to destroy plant cell walls, so that the dissolution and diffusion of substances in cells are facilitated; and the eutectic solvent which has the advantages of no toxicity, biodegradability, recoverability and easy preparation is used as the extractant. Compared with the traditional extraction method, the ultrasonic-assisted eutectic solvent extraction method is a green extraction separation method, improves the extraction efficiency, shortens the extraction time, reduces the use of organic solvents, and is green and environment-friendly.
In addition, the gentiana rigescens of this example is the whole gentiana rigescens. The Chinese pharmacopoeia stipulates that the medicinal parts of gentiana rigescens are roots and rhizomes, and the overground part of the gentiana rigescens is discarded when being harvested. The study shows that the aerial parts of the medicines also contain components such as gentiopicroside, and the contents of the components are not higher than those of underground parts, but the components can be used for substituting the underground parts for the medicines. Along with the deep research and development of the gentiana rigescens, the resource demand is large, so that the whole gentiana rigescens is selected in order to increase the utilization rate of gentiana rigescens resources, reduce the waste treatment of the root and leaves of the gentiana rigescens and change waste into valuable.
In one embodiment, the step of pretreating the whole gentiana rigescens specifically comprises: cleaning whole Gentiana rigescens with water, air drying (optionally air drying), drying at 40-60 deg.C for more than 10 hr, pulverizing, and sieving with 40-80 mesh (such as 60 mesh) pharmacopeia sieve. After the pretreatment is adopted, the obtained gentiana rigescens powder is sealed and stored for later use.
In one embodiment, the method for preparing the eutectic solvent includes the steps of: and mixing the hydrogen bond acceptor and the hydrogen bond donor according to a preset molar ratio, and heating for a preset time under the conditions of a preset temperature and a preset rotating speed to obtain the eutectic solvent.
In one embodiment, the hydrogen bond acceptor may be betaine or the like, and the hydrogen bond donor may be one or two of 1,3-butanediol, urea, glycerol, 1,3-propanediol, lactic acid, or the like.
Betaine is combined with 1,3-butanediol, urea, glycerol, 1,3-propanediol and lactic acid according to a certain molar ratio to form a eutectic solvent, and the solvents are common components in the field of skin care products, so that the composition extract obtained by extraction can be directly used in the skin care products.
When the hydrogen bond donor is selected from two of 1,3-butanediol, urea, glycerol, 1,3-propanediol, lactic acid, etc. (two hydrogen bond donors: hydrogen bond donor 1 and hydrogen bond donor 2), the preparation method of the eutectic solvent comprises the steps of:
mixing a hydrogen bond acceptor and a hydrogen bond donor 1 according to a preset molar ratio, and heating for a preset time under the conditions of a preset temperature and a preset rotating speed to obtain a eutectic solvent 1; mixing the hydrogen bond acceptor and the hydrogen bond donor 2 according to a preset molar ratio, and heating for a preset time under the conditions of a preset temperature and a preset rotating speed to obtain a eutectic solvent 2; and mixing the eutectic solvent 1 and the eutectic solvent 2 to obtain a uniform and transparent eutectic solvent, wherein the eutectic solvent is directly used as an extraction liquid.
In one embodiment, the molar ratio of hydrogen bond acceptor to hydrogen bond donor is 1:2-1.
In one embodiment, the predetermined temperature is 60-90 deg.C, the predetermined time is 30min-2h, and the predetermined rotation speed is 400-800rpm (e.g., 400 rpm). Under this condition, it is possible to ensure that a uniform and transparent eutectic solvent is obtained.
In one embodiment, the mass-to-volume ratio of the gentiana rigescens powder to the eutectic solvent is 1:20-50.
In one embodiment, the time of the ultrasonic treatment is 10-30min, the temperature of the ultrasonic treatment is 40-60 ℃, and the ultrasonic power is 200-500W.
In one embodiment, the step of removing impurities by centrifugation and concentrating specifically comprises: centrifuging at 2000-3000rpm (such as 2000 rpm) to obtain supernatant and residue, extracting the residue with the eutectic solvent for 1-3 times (such as 2 times), collecting supernatant, and concentrating. Wherein the centrifugation time is 10-20min.
The embodiment of the invention provides a radix gentianae extract, which is obtained by extracting with the method for extracting the radix gentianae extract.
The embodiment of the invention provides application of the gentian extract in preparation of cosmetics with sensitive skin repairing efficacy.
The gentian extract obtained in the embodiment of the invention has the effects of resisting inflammation, relieving itching, repairing and the like, and can be directly applied to the field of cosmetics.
The invention is further illustrated by the following specific examples.
Example 1
Cleaning the whole gentiana rigescens with clear water, naturally drying, placing in an oven, drying at 50 ℃ for 12h, crushing by a crusher, sieving by a 60-mesh pharmacopoeia sieve to obtain gentiana rigescens powder, and sealing and storing for later use. Mixing betaine and 1,3-butanediol according to the molar ratio of 1:4, and heating at 80 ℃ and 400rpm for 1h to form a uniform and transparent eutectic solvent. Mixing the gentiana rigescens powder with the prepared eutectic solvent according to the mass volume ratio of 1.
Example 2
Cleaning the whole gentiana rigescens with clear water, naturally drying, placing in an oven, drying at 55 ℃ for 11h, crushing by a crusher, sieving by a 60-mesh pharmacopoeia sieve to obtain gentiana rigescens powder, and sealing and storing for later use. Mixing betaine and glycerol according to the molar ratio of 1:6, and heating at 80 ℃ and 400rpm for 1.5h to form a uniform and transparent eutectic solvent. Mixing the gentiana rigescens powder with the prepared eutectic solvent according to the mass volume ratio of 1.
Example 3
Cleaning the whole gentiana rigescens with clear water, naturally drying, placing in an oven, drying at 60 ℃ for 10h, crushing by a crusher, sieving by a 60-mesh pharmacopoeia sieve to obtain gentiana rigescens powder, and sealing and storing for later use. Mixing betaine and urea according to a molar ratio of 1:4, and heating at 80 ℃ and 400rpm for 2 hours to form a uniform and transparent eutectic solvent 1; mixing betaine and 1,3-butanediol according to the molar ratio of 1:4, and heating at 80 ℃ and 400rpm for 2 hours to form a uniform and transparent eutectic solvent 2; and mixing the eutectic solvent 1 and the eutectic solvent 2 to obtain a uniform and transparent eutectic solvent, wherein the eutectic solvent is directly used as an extraction liquid. Mixing the gentiana rigescens powder with the prepared eutectic solvent according to the mass volume ratio of 1.
The invention also carried out safety and efficacy evaluation tests on the gentian extract obtained in example 3:
example 4
A safety test was performed for example 3:
based on the macrophage cytotoxicity assay, the results are shown in figure 1. As can be seen from fig. 1, the gentian extract obtained in example 3 was macrophage-based, and showed no significant cytotoxicity in the 0.3125% mass concentration range.
Based on the keratinocyte cytotoxicity assay, the results are shown in fig. 2. As can be seen from fig. 2, the gentian extract obtained in example 3 did not exhibit significant cytotoxicity in the mass concentration range of 0.3125% based on keratinocytes.
1. The results of the chick embryo chorioallantoic membrane blood vessel test are shown in Table 1 below.
TABLE 1 toxicity test results of Gentiana scabra Bunge extract on chick embryo chorioallantoic membrane
As can be seen from Table 1 above, the gentian extract was found to be responsible for RC of chick embryo chorioallantoic membrane 50 22.84% (95% CI.
Example 5
The efficacy assessment test was performed for example 3:
1. TNF-alpha inflammatory factor inhibition was tested and the results are shown in FIG. 3. Wherein, BC is a blank control group, NC is a negative control group, and PC (dexamethasone) is a positive control group. When the statistical analysis is carried out by using the 1-test method, compared with the BC group, the significance is represented by #, P-value <0.05 is represented by #, and P-value <0.01 is represented by # #; compared to the NC group, significance is indicated by P-value <0.05 and P-value < 0.01.
And (3) testing results:
compared with a blank control group, the secretion level of TNF-a of the negative control group is obviously increased (P < 0.01), which indicates that the experimental stimulation condition is effective.
Compared with the negative control group, the positive control group has obviously reduced TNF-a secretion level (P < 0.01), which indicates that the positive control group is effective in the experiment.
Compared with a negative control group, the gentian extract can obviously reduce the content of TNF-a.
2. The results of the IL-6 inflammatory factor inhibitory effect test are shown in FIG. 4. Wherein, BC is a blank control group, NC is a negative control group, and PC (dexamethasone) is a positive control group. When the statistical analysis is carried out by using the 1-test method, compared with the BC group, the significance is represented by #, P-value <0.05 is represented by #, and P-value <0.01 is represented by # #; compared to the NC group, significance is indicated by P-value <0.05 and P-value < 0.01.
And (3) testing results:
compared with a blank control group, the IL-6 secretion level of the negative control group is obviously increased (P is less than 0.01), which indicates that the experimental stimulation condition is effective; compared with the negative control group, the IL-6 secretion level of the positive control group is obviously reduced (P is less than 0.01), which indicates that the positive control group is effective in the experiment;
the gentian extract significantly reduced IL-6 levels compared to the negative control group.
Therefore, from the results of examples 4 and 5, it can be seen that the gentian extract has a significant anti-inflammatory effect.
In summary, the invention provides an extraction method of a gentian extract, the gentian extract and application thereof. The method for extracting the gentiana rigescens extract adopts an ultrasonic-assisted extraction technology, utilizes ultrasonic cavitation to destroy plant cell walls, and is beneficial to dissolving and diffusing substances in cells; and the eutectic solvent which has the advantages of no toxicity, biodegradability, recoverability and easy preparation is used as the extractant. Compared with the traditional extraction method, the ultrasonic-assisted eutectic solvent extraction method is a green extraction separation method, improves the extraction efficiency, shortens the extraction time, reduces the use of organic solvents, and is green and environment-friendly. In addition, the invention extracts the whole gentiana rigescens, can increase the utilization rate of gentiana rigescens resources, reduces the waste treatment of the root leaves of gentiana rigescens, and achieves the effect of changing waste into valuables. The gentian extract obtained by the invention has the effects of resisting inflammation, relieving itching, repairing and the like, and can be directly applied to the field of cosmetics.
It is to be understood that the invention is not limited to the examples described above, but that modifications and variations may be effected thereto by those of ordinary skill in the art in light of the foregoing description, and that all such modifications and variations are intended to be within the scope of the invention as defined by the appended claims.
Claims (10)
1. A method for extracting a gentian extract, comprising the steps of:
providing gentian and a eutectic solvent, wherein the gentian is the whole gentiana rigescens;
pretreating the whole gentiana rigescens to obtain gentiana rigescens powder;
mixing the gentiana rigescens powder with a eutectic solvent, carrying out ultrasonic treatment, centrifuging to remove impurities, and concentrating to obtain the gentiana rigescens extract.
2. The method for extracting gentiana rigescens extract as claimed in claim 1, wherein the step of pretreating the whole gentiana rigescens concretely comprises: cleaning the whole Gentiana rigescens with water, air drying, drying at 40-60 deg.C for more than 10 hr, pulverizing, and sieving with 40-80 mesh pharmacopeia sieve.
3. The method of extracting a gentian extract according to claim 1, wherein the method of preparing the eutectic solvent includes the steps of: and mixing the hydrogen bond acceptor and the hydrogen bond donor according to a preset molar ratio, and heating for a preset time under the conditions of a preset temperature and a preset rotating speed to obtain the eutectic solvent.
4. The method for extracting gentian extract as claimed in claim 3, wherein the hydrogen bond acceptor is betaine, and the hydrogen bond donor is one or two of 1,3-butanediol, urea, glycerol, 1,3-propanediol, and lactic acid;
and/or the molar ratio of the hydrogen bond acceptor to the hydrogen bond donor is 1:2-1.
5. The extraction method of gentian extract according to claim 3, wherein the predetermined temperature is 60 to 90 ℃, the predetermined time is 30min to 2 hours, and the predetermined rotation speed is 400 to 800rpm.
6. The extraction method of gentiana rigescens extract as claimed in claim 1, wherein the mass volume ratio of gentiana rigescens powder to eutectic solvent is 1:20-50.
7. The extraction method of gentian extract according to claim 1, wherein the sonication time is 10 to 30min, the sonication temperature is 40 to 60 ℃, and the sonication power is 200 to 500W.
8. The extraction method of the gentian extract according to claim 1, wherein the step of removing impurities by centrifugation and concentrating specifically comprises: centrifuging at 2000-3000rpm to obtain supernatant and residue, extracting the residue with the eutectic solvent for 1-3 times, collecting supernatant, and concentrating.
9. A gentian extract obtained by the extraction method of gentian extract according to any one of claims 1 to 8.
10. Use of the gentian extract according to claim 9 for the preparation of a cosmetic product having sensitive skin repair efficacy.
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CN108904394A (en) * | 2018-09-21 | 2018-11-30 | 广州市科能化妆品科研有限公司 | A kind of Chinese medicine composition and preparation method |
CN113262179A (en) * | 2021-03-19 | 2021-08-17 | 深圳市萱嘉生物科技有限公司 | Plant extract composition with anti-allergy effect and preparation method and application thereof |
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CN108815080A (en) * | 2018-08-21 | 2018-11-16 | 珀莱雅化妆品股份有限公司 | A kind of preparation method of the plant extracts for the black eye that has effects that dispel |
CN108904394A (en) * | 2018-09-21 | 2018-11-30 | 广州市科能化妆品科研有限公司 | A kind of Chinese medicine composition and preparation method |
CN113262179A (en) * | 2021-03-19 | 2021-08-17 | 深圳市萱嘉生物科技有限公司 | Plant extract composition with anti-allergy effect and preparation method and application thereof |
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Application publication date: 20221021 |