CN101554192A - Tea extract-phytosomes composite and preparation method thereof - Google Patents
Tea extract-phytosomes composite and preparation method thereof Download PDFInfo
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Abstract
The invention relates to a tea extract (TE)-phytosomes (ph) composite and a preparation method thereof. The composite takes TE and ph as raw materials. By means of ph encapsulation of the TE, the physical and chemical properties of the TE are changed and the antioxygenic property of the TE in different environments is maintained or enhanced. The invention takes advantage of the ph encapsulation of the TE to change the physical and the chemical properties of the TE and maintain or enhance the antioxygenic property of the TE in different environments, thereby expanding the application approach of the TE and enhancing the functions of the TE in certain environments.
Description
Technical field:
The present invention relates to a kind of tea extract (TE)---phosphatide (phytosomes, compound ph) (TE-ph) and preparation method thereof.
Background technology:
Tea extract mainly contains the active component Tea Polyphenols, has unique anti-oxidant and anti peroxidation of lipid performance, but because Tea Polyphenols tool polyphenol hydroxyl, it is the bigger material of polarity, soluble in water, be insoluble in the oil, and limited its in the grease series products application and bring into play better Human Physiology active function.In addition, because Tea Polyphenols has very strong bitter taste, and also less stable in use, particularly in alkaline environment, very easily oxidized, and lose its distinctive antioxidation, more limited its being extensive use of in food.Moreover, because the Tea Polyphenols quasi-molecule is water-soluble stronger because of it, is difficult in vivo absorb, and greatly reduces its peculiar bioactive bioavilability.
Phosphatide is a kind of phosphorous lipid material, mainly contains phosphatid ylcholine (PC), phosphatidyl-ethanolamine (PE), phosphatidylinositols (PI), serinephosphatide (PS) and phosphatidic acid (PA) etc.Phosphatide is the fundamental component of cell membrane in the animal and plant cells, nuclear membrane and lipid membrane, also is one of composition of nerve cell, and protection, trophic nerve cell are arranged, and accelerates its excited transfer function, and can repair impaired brain cell and neurilemma cell.Natural activity composition and phosphatide are carried out compound under certain condition, obtain natural activity composition phosphatide complexes, can improve effectively in the body of natural activity composition and absorb, improve its bioavilability significantly.
Summary of the invention:
The object of the present invention is to provide a kind of tea extract-phytosomes composite and preparation method thereof, phosphatide embedding by tea extract, with the physicochemical property that changes tea extract and keep or strengthen its antioxygenic property in varying environment, to enlarge the application approach of tea extract, strengthen the effect in some environment.
Technical scheme of the present invention is:
A kind of tea extract-phytosomes composite is characterized in that: it is a raw material with tea extract and phosphatide, by the phosphatide embedding of tea extract, with the physicochemical property that changes tea extract and keep or strengthen its antioxygenic property in varying environment.
Described tea extract-phytosomes composite is characterized in that: total catechin content can 40%～95% in the described tea extract.
Described tea extract-phytosomes composite, it is characterized in that: described phosphatide is that main component is the yolk phospholipid and the soybean lecithin of phosphatid ylcholine, or main component is the cephalin of phosphatidyl-ethanolamine, or the lipositol of main component phosphatidylinositols, or the serinephosphatide of main component phosphatidyl silk amino acid, or the lysophosphatide of main component lysophosphatidyl choline, or comprise the mixture of above-mentioned various phosphatide.
A kind of as the above the preparation method of tea extract-phytosomes composite of claim, it is characterized in that it comprises the steps:
Steps A: raw material phosphatide is added in the non-proton property reaction dissolvent in proportion, and stirring at room, dissolving;
Step B: in tea extract: the mol ratio of phosphatide=1: 0.1～10 adds tea extract gradually to phospholipid solution, heats up gradually, and stirs complex liquid to complex liquid and clarify fully;
Step C: stop to stir, room temperature to be chilled to is filtered, and filtrate is concentrated into a certain amount of, reclaims solvent, puts the vacuum drying chamber vacuum drying again, gets the tea extract-phytosomes composite product;
Solvent and phosphatide ratio in the above-mentioned steps: be 5～200: 1 (V/W).
The preparation method of described tea extract-phytosomes composite, it is characterized in that described non-proton property reaction dissolvent is a kind of in benzinum, n-hexane, cyclohexane, chloroform, dichloroethanes, oxolane, ethyl acetate, ethanol, the benzene, or two or more mixed solvent.
The preparation method of described tea extract-phytosomes composite is characterized in that adding a part in the described non-proton property reaction dissolvent in steps A, adds another part solvent while stirring during stirring in step B.The benefit that substep adds is: decide on the fat-soluble of tea extract raw material and with the ratio of phosphatide, another kind of solvent types and addition need not to add another kind of solvent if single solvent can be made settled solution.
The preparation method of described tea extract-phytosomes composite is characterized in that the intensification temperature described in the step B is 10 ℃～100 ℃.
The preparation method of described tea extract-phytosomes composite is characterized in that the intensification temperature described in the step B is 25 ℃～60 ℃.Reaction temperature is higher than 60 ℃ of raw material instabilities, and active constituent content descends, and oxidation resistance descends, so temperature is low more, and raw material is stable more, descends greatly but be lower than 25 ℃ of reaction dissolvent solubility, and the reaction time prolongs greatly.
The preparation method of described tea extract-phytosomes composite is characterized in that in the steps A raw material phosphatide being put in the three-neck flask of band stirring, thermometer, reflux condensing tube, adds in proportion in the non-proton property reaction dissolvent, and stirring at room, dissolving.
The present invention with the tea extract (TE) of different total polyphenols content as active material, prepare corresponding phosphatide complexes with natural phospholipid, in the prior art of preparation active component phosphatide complexes, its active component all is single chemical drug ingedient, the tea extract-phytosomes composite (TE-ph) of the present invention's preparation, contain various active composition in the tea extract, and its main component catechin, can be the mixture of different content.
The tea extract-phytosomes composite (TE-ph) of preparation active component catechin former with it relatively mainly increases or strengthened the performance of following three aspects:
1. increase the fat-soluble of former active component, thereby increased its use approach.Because by compound active component is the flavone compound that a class contains polyphenol hydroxyl, it is water-soluble stronger and fat-soluble relatively poor, almost insoluble in most of organic solvents, after being prepared into phosphatide complexes, because phosphatide is a kind of amphoteric compound, molecule has a hydrophilic head and two hydrophobic long-chains, wherein hydrophilic segment interacts with active component and combines, and two length fatty acids chains of phosphatide do not participate in recombination reaction, can move freely, the polarity of having wrapped up phosphatide partly forms a lipophilic surface, and it is stronger fat-soluble that compound is shown.
2. increased the stability of former active component in environment for use.Phosphatide complexes is stronger to the stability protection effect of catechin molecule than other amphiphatic molecules.Its protective effect has two aspects, and one is because phosphatide complexes has metastable its fat-soluble increase that combines and make with active component.Make active component be difficult for directly affected by environment and oxidation, it is two because phosphatide is nitrogen-containing compound, and general nitrogen-containing compound can be regenerated as has the antioxidant of removing the free radical effect.
3. increase active component effect in vivo.Phosphatide itself is one of component of cell membrane, the cell membrane of its chemical constituent and human body is approaching, stronger to human body skin and human inner cell's permeability of the membrane, therefore with surface of cell membrane stronger compatibility is arranged, can impel tea extract and cell associative list to reveal and promote to absorb, therefore can improve tea extract through intestines and stomach or Transdermal absorption, can obtain high bioavailability, and active component is eliminated slack-off in vivo, so can improve the bioavilability of tea extract and strengthen its biological action.Phosphatide also is the main constituent of nerve fiber, and along with deepening continuously of biomembrane and nutrition research, the phosphatide conduct is grown and immunity in promotion, lipopenicillinase, and the health-care effect of the anti-ageing aspect of waiting for a long time to be subjected to more common concern approximately.
Description of drawings:
Fig. 1 is that T80 phosphatide complexes (T80-ph) UV scanning is identified collection of illustrative plates;
Fig. 2 is that T90 phosphatide complexes (T90-ph) UV scanning is identified collection of illustrative plates;
Fig. 3 is several fat-soluble antioxidant POV situations of change in time.
The specific embodiment:
The present invention is a raw material with tea extract (TE) and phosphatide (ph).Total catechin content can 40%～95% among the described TE; Described phosphatide can be that main component is the yolk phospholipid and the soybean lecithin of phosphatid ylcholine (Pc), also can be that main component is the cephalin of phosphatidyl-ethanolamine (PE), the lipositol of main component phosphatidylinositols (PI), the serinephosphatide of main component phosphatidyl silk amino acid (Ps) and the lysophosphatide of main component lysophosphatidyl choline (LPC) etc., also can be the mixture that comprises above-mentioned various phosphatide.The main component phosphatid ylcholine in the mixture and the content of phosphatidyl hydramine are on being decided by the difference of composite reactive composition.
The phosphatide cpd preparation must be carried out in non-proton transmission system, and this is that in the solvent of energy ionization, this active force is easy to be broken because the key that phosphatide combines with medicine is an intermolecular force.Active skull cap components generally can not be dissolved in non-proton property reaction dissolvent, but the phosphatide complexes that generates dissolves in this system.
The formation of phosphatide complexes and solvent polarity and consumption thereof, raw material proportioning, temperature, time, charging rate etc. are closely related.The present invention screens with regard to above-mentioned factor, and with desired values such as the difference " Δ A " of UV absorption, apparent oil water partition coefficient " K " value and anti peroxidation of lipid as screening index, but finished tea extract---phosphatide complexes (TE-ph) preparation technology of industrializing implementation.
The concrete preparation technology of product of the present invention is described below:
Material rate: TE: phosphatide=1: 0.1～10 (mol)
Dicyandiamide solution: the dielectric constant of solvent for use system＜25, common solvent has benzinum, n-hexane, cyclohexane, chloroform, dichloroethanes, oxolane, ethyl acetate, ethanol, benzene etc., but the also two or more mixed solvents of dicyandiamide solution single solvent, the ratio between the mixed solvent is by being decided by the character of the active component of compound.
Solvent and phosphatide ratio: generally decide, can be 5～200: 1 (V/W) on solubility, the decentralization of raw material in the preparation dicyandiamide solution
Temperature: the heat endurance and the recombination rate of looking active component are taken all factors into consideration, and can be: 10 ℃～100 ℃.Be generally 25 ℃～60 ℃.
Preparation time: generally determined by the association rate and the factors such as solubility of phosphatide complexes in system of solubility, decentralization, mixing speed, active component and the phosphatide of raw material in the preparation dicyandiamide solution.Can be: 30 minutes～50 hours.Be generally 2 hours～12 hours.
The phosphatide complexes preparation process is as follows:
1. raw material phosphatide is put in the three-neck flask of band stirring, thermometer, reflux condensing tube, added the dissolving of system solvent orange 2 A stirring at room in proportion.
2. in proportion (1: 0.1～10) add TE gradually to phospholipid solution, but powder add, add after the also available an amount of dissolution with solvents, be warming up to gradually and require temperature, stir complex liquid on request to certain hour.
3. limit during stirring, stir the limit on request ratio gradually gradation add solvent B, continue to be stirred to complex liquid and clarify fully.
4. stop to stir, room temperature to be chilled to is filtered, and filtrate is concentrated into a certain amount of, reclaims solvent, puts the vacuum drying chamber vacuum drying again, gets tea extract-phytosomes composite (TE-ph) product.
Annotate: dicyandiamide solution A and solvent B, can add simultaneously, also as above step adds, and decides on the recombination reaction situation.
The structure of tea extract-phytosomes composite, liposoluble performance and antioxygenic property
1. tea extract-phytosomes composite and tea extract UV absorption difference are relatively
Stronger interaction has taken place with active component and has formed in the polar group part of phosphatide complexes phosphatide, therefore there is the spectral signature of the active component of UV absorption to change to some extent, the absorption value of ultimate constituent can reduce, estimating the integrality of phosphatide composite reactive composition with former active component and active component phosphatide complexes in the difference of the absorption value of ultraviolet absorption peak, also is one of evaluation criterion of phosphatide complexes.Referring to honesty, Wang Baichu " biotechnology communication " .Vol:17No:830～833
Test specimen:
1. the raw material for preparing TE-ph: tea extract T90 and T80 (total catechin content is respectively 90% and 80%);
2. with the TE soybean lecithin compound T80-ph and the T90-ph of above-mentioned feedstock production.The ratio of prepared sample its raw material T90 and T80 and phosphatide all is: raw material TE: phosphatide=1: 1 (mol ratio).
Be dissolved in each sample in the ethyl acetate respectively, all be mixed with respectively with TE concentration is the 0.1mgTE/ml ethyl acetate solution of benchmark, be that T90 concentration and the T80 among T80 and the T80-ph among T90 and the T90-ph is 0.1mg/ml, in the ratio of TE raw material and phosphatide, then T90-ph and the T80-ph concentration in solution all is 0.26mg/ml.Phospholipid concentration 0.16mg/ml wherein.
Fig. 1 and Fig. 2 are respectively T90-ph and T80-ph UV scanning collection of illustrative plates, scintigram shows, two samples all have the strongest absworption peak at the 270nm place, and the soybean lecithin solution of respective concentration 270nm do not have absworption peak (annotate: when measuring TE and TE-ph respectively the soybean lecithin ethyl acetate solution with ethyl acetate and respective concentration be blank).Because the shielding action of phosphatide, the catechin absorption value of TE-ph reduces.
It is Δ A=3.18-2.02=1.16 that T80 and T80-ph absorb value difference at the 270nm place;
It is Δ A=3.40-2.53=0.87 that T90 and T90-ph absorb value difference at the 270nm place.
2. liposoluble performance---apparent oil water partition coefficient K value
Active component is after phosphatide is compound, and common fat-soluble meeting strengthens, and the apparent oil water partition coefficient is with this fat-soluble enhanced propertied datumization.
Test specimen is T90, T90-ph.Taking by weighing T90 and T90-ph 0.01g respectively also is dissolved in respectively in a certain amount of distilled water and the fat organic solvent, in the T90 aqueous solution and T90-ph fat organic solvent solution, add equivalent fat organic solvent and distilled water more respectively, leave standstill after the jolting, catechin component distributes automatically at ethyl acetate and aqueous phase in the sample, separate two phase liquid, respectively with the coordinative solvent constant volume.Carry out high pressure liquid phase (HPLC) chromatography and detect wherein catechin content, divided by the aqueous phase catechin content, the numerical value that obtains is K value (K with the middle mutually catechin content of fat
Fat phase/water), the K value is big more to show fat-soluble strong more (being water-soluble poor more).
Used fat organic solvent is respectively ethyl acetate and chloroform in the test
Table 1 apparent oil water partition coefficient
Table 1 data show: the K of T90-ph
Ethyl Acetate/waterAnd K
Chloroform/waterValue is much larger than the K of T90
Ethyl Acetate/waterAnd K
Chloroform/waterValue shows its fat-soluble increase greatly of tea extract (TE) after phosphatide is compound.And the fat solvent polarity is more little, and the K value of T90 and T90-ph differs big more.Show that also T90-ph has very wide solubilized scope in the fat solvent.
3. to the inhibiting rate of hexichol for bitter taste hydrazine free radical (DPPH)
Free radical is meant to have and does not match atom, atomic group or the molecule of valence electron.Most of free-radical chemistry character are very active, and the life-span is extremely short.And hexichol for bitter taste diazanyl free radical (DPPH) because the spatial obstacle of three phenyl ring is arranged, be clipped in the middle of it unpaired electron on nitrogen-atoms and can not bring into play its due electronics and act in pairs and make, so a stable free radical can be provided.And DPPH has the last one to absorb at the 517nm place, its ethanolic solution is darkviolet.When free radical scavenger existed, owing to its single electron pairing its absorption being faded away, its fading extent became quantitative relationship with the electron amount of its acceptance.Thereby available optical spectroscopy carries out quantitative analysis.
Test specimen: T80, T80-ph, Rosmarinus officinalis extract, sample specification sees Table 2.
Condition determination: quality such as all samples are dissolved in the ethanol, concentration: 25ppm (0.025mg/ml); DPPH concentration: 300 μ mol/L; Measure wavelength: 517nm.
Do the sample blank contrast with the ethanol that does not add sample solution during mensuration.
Assay method is referring to following two pieces of documents: (1) Chen Jiwu, Hu Bin, Zhao Shi etc., luminous journal, the 26th the 5th phase of volume, in October, 2005: 664-668; (2) Li Hong, Zhang Yuanhu uses the oxidation resistance that the DPPH method is measured apple extract, Shandong Agricultural University's journal (natural science edition), the 36th the 1st phase of volume: 35～38.
Table 2: test specimen specification and inhibiting rate
| Sample | Sample size % (EGCG/ total polyphenols) | Inhibiting rate % |
| T80 | 61.0/80.0 | 94.1 |
| T80-ph | 23.19/30.23 | 50.0 |
| Rosmarinus officinalis extract | Carnosic acid content 〉=60% | 53.0 |
As can be known from Table 2, sample is relevant with total catechin content substantially to the DPPH inhibiting rate.In view of the above, total catechin content ratio of pressing T80 and T80-ph, phosphatide complexes is not only sheltered the free radical inhibitory action of catechin self, and has strengthened this effect.
4. anti-grease lipid peroxidation performance (grease lipid peroxidation value POV mensuration)
Generate peroxide in the Oxidation of Fat and Oils process, peroxide and KI effect generate free-iodine, with sodium thiosulfate solution titrated, calculate the content of generation peroxide with the volume of titration.When containing antioxidant in the oil, the amount of the peroxide of its generation just reduces, and promptly the POV value just reduces, and judges the performance quality of antioxidant with POV value height.
Assay method is measured with reference to GB5009.37-1996.
Working sample and specification see Table 3
Condition determination: wait quality to be dissolved in the soybean oil of no TBHQ respectively in table 3 sample, put under 98 ℃ of conditions and be incubated accelerated oxidation, different time sections (hour): 0,4,8,12,16,22,28,32,52,70,78, measure grease matter peroxide value (POV, the unit: meq/kg) of each sample.
Sample concentration: 100ppm (0.1mg sample/ml soybean oil).
Table 3: test specimen specification
| Sample | Content % |
| T80 (EGCG/ total polyphenols) | 61.0/80.0 |
| T80-ph (EGCG/ total polyphenols) | 23.19/30.23 |
| The ether fragrant extract (carnosic acid content) that changes | ≥60 |
| Ve (total tocopherol content) | ≥90 |
Fig. 3 result shows, waits the stability of the anti-oil peroxidation of quality sample to be followed successively by from high to low: T80-ph＞ether fragrant extract＞T80 ≈ Ve that changes.At 98 ℃, 78 hours ends, the POV value of T80-ph significantly is lower than other three kinds of fat-soluble antioxidants.See accompanying drawing 3.In addition, with regard to T80-ph and T80 anti peroxidation of lipid performance, antioxygenic property is not exclusively relevant with total catechin in grease, T80-PH shown phosphatide in vegetable oil is anti-oxidant stablize and repair.
Embodiment
Embodiment one
Get soybean lecithin 15 gram and put in the three-neck flask, add the dissolving of chloroform 200ml stirring at room after, add TE (total catechin content 80%) 10 grams while stirring gradually, be warming up to 40 ℃ gradually, stir after 2 hours, add absolute ethyl alcohol 20ml while stirring gradually, continue to stir solution clarification after 2 hours.The filtered and recycled solvent, vacuum drying gets tea extract-phytosomes composite (TE-ph) product.
Embodiment two
Get lecithin 16 grams and put in the three-neck flask, add the dissolving of benzinum 350ml stirring at room.Other gets TE10 gram (total catechin content 80%), adds gradually in the benzinum phospholipid solution, is warming up to 40 ℃ gradually, stirs after 2 hours, adds absolute ethyl alcohol 20ml while stirring gradually, continues to stir solution clarification after 1 hour.The filtered and recycled solvent, vacuum drying gets the TE-ph product.
Embodiment three
Get soybean lecithin 45 grams and put in the three-neck flask, add the dissolving of chloroform 900ml stirring at room.Other gets TE27 gram (total catechin content 50%), adds gradually while stirring in the chloroform phospholipid solution, is warming up to 60 ℃ gradually, stirs after 2 hours, adds absolute ethyl alcohol 50ml while stirring gradually, and 40 ℃ are continued to stir solution clarification after 2 hours down.The filtered and recycled solvent, vacuum drying gets the TE-ph product.
Embodiment four
Get lecithin 20 grams and put in the three-neck flask, add the dissolving of benzinum 400ml stirring at room.Other gets TE10 gram (total catechin content 50%), adds gradually in the benzinum phospholipid solution, is warming up to 60 ℃ gradually, stirs after 2 hours, adds absolute ethyl alcohol 25ml while stirring gradually, continues to stir solution clarification after 1 hour.The filtered and recycled solvent, vacuum drying gets the TE-ph product.
Embodiment five
Get lecithin 40 grams and put in the three-neck flask, add the dissolving of chloroform 3800ml stirring at room.Other gets TE20 gram (total catechin content 90%), behind the 600ml acetic acid ethyl dissolution, adds gradually in the chloroform phospholipid solution, is warming up to 35 ℃ gradually, stirs after 5 hours, adds absolute ethyl alcohol 15ml while stirring gradually, and 35 ℃ are continued to stir 1 hour, the solution clarification.The filtered and recycled solvent, vacuum drying gets the TE-ph product.
Embodiment six
Get lecithin 32 grams and put in the three-neck flask, add the dissolving of benzinum 3000ml stirring at room.Other gets TE23 gram (total catechin content 90%), behind 200ml ethyl acetate+10 anhydrous alcohol solutions, adds gradually in the benzinum phospholipid solution, is warming up to 35 ℃ gradually, stirs solution clarification after 5 hours.The filtered and recycled solvent, vacuum drying gets the TE-ph product.
Being preferred embodiment of the present invention only in sum, is not to be used for limiting practical range of the present invention.Be that all equivalences of doing according to the content of the present patent application claim change and modification, all should be technology category of the present invention.
Claims (9)
1, a kind of tea extract-phytosomes composite is characterized in that: it is a raw material with tea extract and phosphatide, by the phosphatide embedding of tea extract, with the physicochemical property that changes tea extract and keep or strengthen its antioxygenic property in varying environment.
2, tea extract-phytosomes composite according to claim 1 is characterized in that: total catechin content can 40%～95% in the described tea extract.
3, tea extract-phytosomes composite according to claim 1, it is characterized in that: described phosphatide is that main component is the yolk phospholipid and the soybean lecithin of phosphatid ylcholine, or main component is the cephalin of phosphatidyl-ethanolamine, or the lipositol of main component phosphatidylinositols, or the serinephosphatide of main component phosphatidyl silk amino acid, or the lysophosphatide of main component lysophosphatidyl choline, or comprise the mixture of above-mentioned various phosphatide.
4, a kind of preparation method as claim 1 or 2 or 3 described tea extract-phytosomes composites is characterized in that it comprises the steps:
Steps A: raw material phosphatide is added in the non-proton property reaction dissolvent in proportion, and stirring at room, dissolving;
Step B: in tea extract: the mol ratio of phosphatide=1: 0.1～10 adds tea extract gradually to phospholipid solution, heats up gradually, and stirs complex liquid to complex liquid and clarify fully;
Step C: stop to stir, room temperature to be chilled to is filtered, and filtrate is concentrated into a certain amount of, reclaims solvent, puts the vacuum drying chamber vacuum drying again, gets the tea extract-phytosomes composite product;
Solvent and phosphatide ratio in the above-mentioned steps: be 5～200: 1 (V/W).
5, the preparation method of tea extract-phytosomes composite according to claim 4, it is characterized in that described non-proton property reaction dissolvent is a kind of in benzinum, n-hexane, cyclohexane, chloroform, dichloroethanes, oxolane, ethyl acetate, ethanol, the benzene, or two or more mixed solvent.
6, the preparation method of tea extract-phytosomes composite according to claim 4 is characterized in that adding a part in the described non-proton property reaction dissolvent in steps A, adds another part solvent while stirring during stirring in step B.
7, the preparation method of tea extract-phytosomes composite according to claim 4 is characterized in that the intensification temperature described in the step B is 10 ℃～100 ℃.
8, the preparation method of tea extract-phytosomes composite according to claim 7 is characterized in that the intensification temperature described in the step B is 25 ℃～60 ℃.
9, the preparation method of tea extract-phytosomes composite according to claim 4, it is characterized in that in the steps A raw material phosphatide being put in the three-neck flask of band stirring, thermometer, reflux condensing tube, add in proportion in the non-proton property reaction dissolvent, and stirring at room, dissolving.
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| CN111035696A (en) * | 2019-12-16 | 2020-04-21 | 格律药业有限公司 | Pharmaceutical composition containing tea extract and its use for treating cancer |
| CN111084387A (en) * | 2019-12-24 | 2020-05-01 | 李晨悦 | Multifunctional nutritional composition, preparation method thereof and health food |
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