CN106866998A - A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel and its preparation method and application - Google Patents
A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel and its preparation method and application Download PDFInfo
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Abstract
The invention belongs to functional high molecule material and biology medical material technical field, and in particular to a kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel and its preparation method and application.It with chitosan quaternary ammonium salt and carboxymethylcellulose calcium is polysaccharide raw material that the superabsorbent hydrogel is, the citric acid with safety non-toxic as crosslinking agent, as obtained by prepared by cross-linking reaction.Wherein, chitosan quaternary ammonium salt accounts for the 10%~50% of polysaccharide raw material gross mass, and carboxymethylcellulose calcium accounts for the 50%~90% of polysaccharide raw material gross mass.Superabsorbent hydrogel of the present invention is respectively provided with excellent swelling behavior for pure water, physiological saline, glucose solution, urea liquid and synthesis urine；Additionally, also having excellent anti-microbial property.Environmental protection of the present invention, process is simple, low production cost is expected to use it for bio-medical and personal hygiene material.
Description
Technical field
The invention belongs to Functional polymer materials technology field, biomedical materials field is fallen within, and in particular to a kind of
Chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel and its preparation method and application.
Background technology
In recent years, the advantages of superabsorbent hydrogel (resin) is because of its high swelling property, pH sensitiveness and good water retention property, quilt
It is widely used in every field, such as agricultural, hygienic material, sewage disposal, pharmaceutical carrier, organizational project and heavy metal adsorption.
The market demand of superabsorbent hydrogel is huge, and what is be most widely used at present is synthesis material class, mainly with acrylic acid and acryloyl
Superabsorbent hydrogel prepared by the homopolymerization of the monomer such as amine or copolymerization.The superabsorbent hydrogel typically has good water absorbing properties, however, its
Biological degradability is not enough.Therefore, in recent years, biodegradable superabsorbent hydrogel turns into one of important development trend.Wherein,
The superabsorbent hydrogel of natural polysaecharides receives extensive concern, such as cellulose and shitosan, and it not only has good biology
Degradability, and production cost can be significantly reduced.
Carboxymethylcellulose calcium (Carboxymethyl Cellulose) is a kind of anionic cellulose ether, is research at present
At most, most widely used a kind of cellulose derivative.It is water-soluble poor due to its acid, thus carboxymethylcellulose calcium it is general with
The form of sodium salt is present.The application of carboxymethylcellulose calcium is widely：In food industry, carboxymethylcellulose calcium mainly rise thickening,
Stabilization, water conservation etc. are acted on；In medicine, carboxymethylcellulose calcium to medicine, protein etc. with good compatibility and load capacity,
And with good biocompatibility, so often by as pharmaceutical carrier；Carboxymethyl cellulose gel also possesses good mechanics
Performance and pH sensitiveness, often by the material as tissue engineering bracket.
Shitosan (Chitosan) is a kind of natural alkaline polysaccharide, with good biodegradability, biocompatibility
With reactivity etc..But due to there are a large amount of hydrogen bond actions with intermolecular in chitosan molecule, its dissolubility is poor so that shell gathers
Sugared is of limited application.Chitosan quaternary ammonium salt can introduce quaternary ammonium salt group and be prepared from by N in shitosan, its preparation
Method is simple, low cost.Used as a kind of cationic chitosan derivative, chitosan quaternary ammonium salt not only has the advantages that shitosan,
Also there is good dissolubility and antibiotic property.
The preparation of superabsorbent hydrogel generally uses chemical cross-linking agent, and the crosslinking agent such as aldehydes commonly used at present has itself
Toxicity and safety issue, cause its application in the field such as bio-medical and personal hygiene material to be restricted.
The content of the invention
The present invention is in view of the shortcomings of the prior art, it is therefore intended that provide a kind of (raw with excellent water suction, suction physiological solution
Reason salt solution, glucose solution, urea liquid, synthesis urine solution) and the chitosan quaternary ammonium salt/carboxymethylcellulose calcium of anti-microbial property it is super
Water absorbent gel and its preparation method and application.
For achieving the above object, the technical solution adopted by the present invention is：
A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, by chitosan quaternary ammonium salt and carboxymethylcellulose calcium
Two kinds of polysaccharide raw materials are prepared from the presence of crosslinking agent, wherein, chitosan quaternary ammonium salt accounts for the 10% of polysaccharide raw material gross mass
~50%, carboxymethylcellulose calcium accounts for the 50%~90% of polysaccharide raw material gross mass.
In such scheme, the chitosan quaternary ammonium salt is HACC.
In such scheme, the crosslinking agent is citric acid.
In such scheme, the consumption of the crosslinking agent for chitosan quaternary ammonium salt and carboxymethylcellulose calcium gross mass 3%~
30%.
The preparation method of above-mentioned chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, comprises the following steps：
(1) chitosan quaternary ammonium salt is dissolved in appropriate distilled water, stirring is to being completely dissolved；It is subsequently adding carboxymethyl cellulose
Element, stirs, and obtains the composite solution of chitosan quaternary ammonium salt and carboxymethylcellulose calcium；
(2) to citric acid solution is added in step (1) gained composite solution, stir, obtain chitosan quaternary ammonium salt, carboxylic
The mixed solution of methylcellulose and citric acid, isothermal reaction is for a period of time under mixed solution is placed in into uniform temperature；
(3) after reaction terminates, respectively with deionized water and ethanol detergent gel, gel obtains shell and gathers after drying, that is, again
Sugared quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel.
In such scheme, the concentration of carboxymethylcellulose calcium is 2.5%~5.5% in the mixed solution.
In such scheme, described the stirring of step (2) carried out under the conditions of 30 DEG C.
In such scheme, the temperature of step (2) described isothermal reaction is 85 DEG C, and the time is 3 hours.
In such scheme, step (3) described drying is freeze-drying or drying, and the temperature of the drying is less than 60 DEG C.
Above-mentioned chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel is in bio-medical and personal hygiene Material Field
Using.
Beneficial effects of the present invention：
(1) present invention, using citric acid as crosslinking agent, is prepared into chitosan quaternary ammonium salt and carboxymethylcellulose calcium as base material
To a kind of new superabsorbent hydrogel (chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel), the chitosan quaternary ammonium salt/carboxylic
Methylcellulose superabsorbent hydrogel is respectively provided with excellent for pure water, physiological saline, glucose solution, urea liquid and synthesis urine
Swelling behavior, while also having excellent antibacterial characteristics；
(2) base material used by superabsorbent hydrogel of the present invention is biodegradable natural polysaccharide, and crosslinking agent used is green
The nontoxic citric acid of color, does not result in environmental pollution, meets the requirement of environmental protection and sustainable development.Based on the safe nothing of raw material
Poison, therefore, chitosan quaternary ammonium salt of the present invention/carboxymethylcellulose calcium superabsorbent hydrogel can be used for bio-medical and personal hygiene
Material Field；
(3) superabsorbent hydrogel of the present invention is for pure water, physiological saline, glucose solution, urea liquid and synthesis urine
Swelling behavior, and anti-microbial property all can be according to different use needs, by adjusting chitosan quaternary ammonium salt, carboxymethylcellulose calcium
Concentration etc. with the consumption of citric acid, and carboxymethylcellulose calcium is regulated and controled, to adapt to different application demands；
(4) raw materials used wide material sources of the invention are easy to get, low cost, and preparation process is simple is expected to realize commercial application,
And the product huge market demand.
Brief description of the drawings
Fig. 1 is that the preparation of chitosan quaternary ammonium salt of the present invention/carboxymethylcellulose calcium superabsorbent hydrogel and microstructure are shown
It is intended to.
Fig. 2 is the scanning electron microscope (SEM) photograph of chitosan quaternary ammonium salt of the present invention/carboxymethylcellulose calcium superabsorbent hydrogel.
Specific embodiment
For a better understanding of the present invention, it is with reference to the embodiment content that the present invention is furture elucidated but of the invention
Content is not limited solely to the following examples.
Embodiment 1
A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, is prepared via a method which to obtain：
(1) by a certain amount of chitosan quaternary ammonium salt, (consumption is two kinds of total matter of polysaccharide of chitosan quaternary ammonium salt and carboxymethylcellulose calcium
20%) amount is dissolved in appropriate distilled water, and stirring is to being completely dissolved；(consumption is chitosan quaternary ammonium to add carboxymethylcellulose calcium
Two kinds of polysaccharide gross mass of salt and carboxymethylcellulose calcium 80%), stir, obtain chitosan quaternary ammonium salt and carboxymethyl fine
Tie up the composite solution of element；
(2) to step (1) gained composite solution addition citric acid solution, (Citric Acid Dosage is chitosan quaternary ammonium salt and carboxylic first
Two kinds of polysaccharide gross mass of base cellulose 10%), stirred in 30 DEG C, obtain chitosan quaternary ammonium salt, carboxymethylcellulose calcium and
The mixed solution of citric acid, carboxymethylcellulose calcium concentration is 4% in the mixed solution；
(3) and then, by the mixed solution of above-mentioned gained in 85 DEG C of isothermal reactions 3 hours；
(4) after reaction terminates, gel is washed with deionized water and ethanol respectively, after being dried in 45 DEG C, obtains shitosan
Quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel.
The swelling behavior of superabsorbent hydrogel is tested using weight method, swellbility is calculated by formula (1)：
W0It is the initial mass (g) before dry state superabsorbent swelling behavior, WeWeight when being balanced for superabsorbent swelling behavior
(g)。
The present embodiment prepares chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel and the swellbility of pure water is reached
535g/g, the result shows that the superabsorbent hydrogel has excellent water absorbing properties.
The preparation of the chitosan quaternary ammonium salt that Fig. 1 is prepared for the present embodiment/carboxymethylcellulose calcium superabsorbent hydrogel and micro-
See structural representation.Shown in figure, using the hydroxyl on citric acid cross-linked chitosan quaternary ammonium salt and carboxymethylcellulose calcium strand
It is prepared for a kind of new superabsorbent hydrogel.Chitosan quaternary ammonium salt of the present invention/carboxymethylcellulose calcium superabsorbent hydrogel section
Scanning electron microscope (SEM) photograph is as shown in fig. 2, it can be seen that the compatibility of chitosan quaternary ammonium salt and carboxymethylcellulose calcium is good, and forms
Complete cross-linked network structure, shows that the superabsorbent hydrogel is successfully prepared.
Embodiment 2
A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, is prepared via a method which to obtain：
(1) by a certain amount of chitosan quaternary ammonium salt, (consumption is two kinds of total matter of polysaccharide of chitosan quaternary ammonium salt and carboxymethylcellulose calcium
20%) amount is dissolved in appropriate distilled water, and stirring is to being completely dissolved；(consumption is chitosan quaternary ammonium to add carboxymethylcellulose calcium
Two kinds of polysaccharide gross mass of salt and carboxymethylcellulose calcium 80%), stir, obtain chitosan quaternary ammonium salt and carboxymethyl fine
Tie up the composite solution of element；
(2) to the citric acid solution of addition set amount in step (1) gained composite solution, (Citric Acid Dosage is shitosan season
Two kinds of polysaccharide gross mass of ammonium salt and carboxymethylcellulose calcium 3%), stirred in 30 DEG C, obtain chitosan quaternary ammonium salt, carboxymethyl
The mixed solution of cellulose and citric acid, carboxymethylcellulose calcium concentration is 4% in the mixed solution；
(3) and then, by the mixed solution of above-mentioned gained in 85 DEG C of isothermal reactions 3 hours；
(4) after reaction terminates, gel is washed with deionized water and ethanol respectively, chitosan quaternary ammonium is obtained after freeze-drying
Salt/carboxymethylcellulose calcium superabsorbent hydrogel.
The present embodiment prepares chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel in physiological saline (0.9% chlorine
Change sodium) distinguish with the swellbility in synthesis urine solution (0.8% sodium chloride, 0.1% magnesium sulfate, 2% urea, 0.06% calcium chloride)
It is 68g/g and 51g/g, as a result shows that the superabsorbent hydrogel has good swellability for physiological saline and synthesis urine solution
Energy.
Embodiment 3
A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, is prepared via a method which to obtain：
(1) by a certain amount of chitosan quaternary ammonium salt, (consumption is two kinds of total matter of polysaccharide of chitosan quaternary ammonium salt and carboxymethylcellulose calcium
20%) amount is dissolved in appropriate distilled water, and stirring is to being completely dissolved；(consumption is chitosan quaternary ammonium to add carboxymethylcellulose calcium
Two kinds of polysaccharide gross mass of salt and carboxymethylcellulose calcium 80%), stir, obtain chitosan quaternary ammonium salt and carboxymethyl fine
Tie up the composite solution of element；
(2) to the citric acid solution of addition set amount in step (1) gained composite solution, (Citric Acid Dosage is shitosan season
Two kinds of polysaccharide gross mass of ammonium salt and carboxymethylcellulose calcium 10%), stirred in 30 DEG C, obtain chitosan quaternary ammonium salt, carboxylic first
The mixed solution of base cellulose and citric acid, carboxymethylcellulose calcium concentration is 2.5% in the mixed solution；
(3) and then, by the mixed solution of above-mentioned gained in 85 DEG C of isothermal reactions 3 hours；
(4) after reaction terminates, gel is washed with deionized water and ethanol respectively, is dried (temperature of drying is less than 60 DEG C)
After obtain chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel.
The present embodiment prepares chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel in glucose solution (concentration
5%) swellbility in reaches 512g/g, as a result shows that the superabsorbent hydrogel has excellent swelling behavior for glucose solution.
Embodiment 4
A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, is prepared via a method which to obtain：
(1) by a certain amount of chitosan quaternary ammonium salt, (consumption is two kinds of total matter of polysaccharide of chitosan quaternary ammonium salt and carboxymethylcellulose calcium
20%) amount is dissolved in appropriate distilled water, and stirring is to being completely dissolved；(consumption is chitosan quaternary ammonium to add carboxymethylcellulose calcium
Two kinds of polysaccharide gross mass of salt and carboxymethylcellulose calcium 80%), stir, obtain chitosan quaternary ammonium salt and carboxymethyl fine
Tie up the composite solution of element；
(2) to the citric acid solution of addition set amount in step (1) gained composite solution, (Citric Acid Dosage is shitosan season
Two kinds of polysaccharide gross mass of ammonium salt and carboxymethylcellulose calcium 10%), stirred in 30 DEG C, obtain chitosan quaternary ammonium salt, carboxylic first
The mixed solution of base cellulose and citric acid, carboxymethylcellulose calcium concentration is 3% in the mixed solution；
(3) and then, by the mixed solution of above-mentioned gained in 85 DEG C of isothermal reactions 3 hours；
(4) reaction terminate after, gel is washed with deionized water and ethanol respectively, drying after obtain chitosan quaternary ammonium salt/
Carboxymethylcellulose calcium superabsorbent hydrogel.
The present embodiment prepares chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel in urea liquid (concentration
5%) swellbility in reaches 332g/g, as a result shows that the superabsorbent hydrogel has good swelling behavior for urea liquid.
Embodiment 5
A kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, is prepared via a method which to obtain：
(1) by a certain amount of chitosan quaternary ammonium salt, (consumption is two kinds of total matter of polysaccharide of chitosan quaternary ammonium salt and carboxymethylcellulose calcium
40%) amount is dissolved in appropriate distilled water, and stirring is to being completely dissolved；(consumption is chitosan quaternary ammonium to add carboxymethylcellulose calcium
Two kinds of polysaccharide gross mass of salt and carboxymethylcellulose calcium 60%), stir, obtain chitosan quaternary ammonium salt and carboxymethyl fine
Tie up the composite solution of element；
(2) to the citric acid solution of addition set amount in step (1) gained composite solution, (Citric Acid Dosage is shitosan season
Two kinds of polysaccharide gross mass of ammonium salt and carboxymethylcellulose calcium 10%), stirred in 30 DEG C, obtain chitosan quaternary ammonium salt, carboxylic first
The mixed solution of base cellulose and citric acid, carboxymethylcellulose calcium concentration is 4% in the mixed solution；
(3) and then, by the composite solution of above-mentioned gained in 85 DEG C of isothermal reactions 3 hours；
(4) reaction terminate after, gel is washed with deionized water and ethanol respectively, drying after obtain chitosan quaternary ammonium salt/
Carboxymethylcellulose calcium superabsorbent hydrogel.
The anti-microbial property of superabsorbent hydrogel is tested using absorbance method, bacteriostasis rate is calculated by formula (2)：
A is the bacteria culture media absorbance for adding superabsorbent hydrogel, A0For the bacteria culture media for not adding superabsorbent hydrogel is inhaled
Luminosity.
The present embodiment prepares the anti-microbial property result table of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel
Bright, the bacteriostasis rate to staphylococcus aureus (gram-positive bacteria) reaches 97%, to Escherichia coli (Gram-negative bacteria)
Bacteriostasis rate reaches 51%.
Obviously, above-described embodiment is only intended to clearly illustrate made example, and not to the limitation of implementation method.It is right
For those of ordinary skill in the art, can also make on the basis of the above description other multi-forms change or
Change.There is no need and unable to be exhaustive to all of implementation method.And the obvious change or change therefore amplified
Move within still in the protection domain of the invention.
Claims (9)
1. a kind of chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel, it is characterised in that the superabsorbent hydrogel is by shell
Two kinds of polysaccharide raw materials of glycan quaternary ammonium salt and carboxymethylcellulose calcium are prepared from the presence of crosslinking agent, wherein, chitosan quaternary ammonium
Salt accounts for the 10% ~ 50% of polysaccharide raw material gross mass, and carboxymethylcellulose calcium accounts for the 50% ~ 90% of polysaccharide raw material gross mass.
2. chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel according to claim 1, it is characterised in that the shell
Glycan quaternary ammonium salt is HACC.
3. chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel according to claim 1, it is characterised in that the friendship
Connection agent is citric acid.
4. chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel according to claim 1, it is characterised in that the friendship
The consumption for joining agent is the 3% ~ 30% of chitosan quaternary ammonium salt and carboxymethylcellulose calcium gross mass.
5. the preparation method of any chitosan quaternary ammonium salt of claim 1 ~ 4/carboxymethylcellulose calcium superabsorbent hydrogel, its feature
It is to comprise the following steps：
（1）Chitosan quaternary ammonium salt is dissolved in appropriate distilled water, stirring is to being completely dissolved；Carboxymethylcellulose calcium is subsequently adding, is filled
Divide and stir, obtain the composite solution of chitosan quaternary ammonium salt and carboxymethylcellulose calcium；
（2）To step（1）Citric acid solution is added in gained composite solution, is stirred, obtain chitosan quaternary ammonium salt, carboxymethyl
The mixed solution of cellulose and citric acid, isothermal reaction is for a period of time under mixed solution is placed in into uniform temperature；
（3）After reaction terminates, respectively with deionized water and ethanol detergent gel, gel obtains shitosan season after drying, that is, again
Ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel.
6. preparation method according to claim 5, it is characterised in that the concentration of carboxymethylcellulose calcium in the mixed solution
It is 2.5% ~ 5.5%.
7. preparation method according to claim 5, it is characterised in that step（2）The temperature of the isothermal reaction is 85 DEG C,
Time is 3 hours.
8. preparation method according to claim 5, it is characterised in that step（3）The drying be freeze-drying or drying,
The temperature of the drying is less than 60 DEG C.
9. any chitosan quaternary ammonium salt/carboxymethylcellulose calcium superabsorbent hydrogel of claim 1 ~ 4 is in bio-medical and individual
The application in hygienic material field.
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|---|---|---|---|---|
| CN108047379A (en) * | 2017-12-28 | 2018-05-18 | 四川大学 | A kind of preparation method of temperature-sensitive hydrogel |
| CN108939056A (en) * | 2018-07-25 | 2018-12-07 | 张河 | A kind of biological polyoses rinse glue and preparation method thereof |
| CN109512579A (en) * | 2018-10-08 | 2019-03-26 | 武汉纺织大学 | A kind of multilayer moisture absorption is breathed freely magnetic therapy and intelligent temperature control type dressing and application method |
| CN110294522A (en) * | 2019-05-23 | 2019-10-01 | 浙江理工大学 | A kind of preparation method handling dyeing waste water both sexes flocculation material |
| CN112375260A (en) * | 2020-11-17 | 2021-02-19 | 齐鲁工业大学 | Preparation method of glucose-based porous water-absorbing edible gel |
| CN112625306A (en) * | 2021-01-11 | 2021-04-09 | 中国制浆造纸研究院有限公司 | Full-biodegradable water-absorbent resin and preparation method thereof |
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Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108047379A (en) * | 2017-12-28 | 2018-05-18 | 四川大学 | A kind of preparation method of temperature-sensitive hydrogel |
| CN108939056A (en) * | 2018-07-25 | 2018-12-07 | 张河 | A kind of biological polyoses rinse glue and preparation method thereof |
| CN109512579B (en) * | 2018-10-08 | 2022-02-18 | 武汉纺织大学 | Multi-layer moisture-absorption breathable magnetic therapy and intelligent temperature control type dressing and using method |
| CN109512579A (en) * | 2018-10-08 | 2019-03-26 | 武汉纺织大学 | A kind of multilayer moisture absorption is breathed freely magnetic therapy and intelligent temperature control type dressing and application method |
| CN110294522A (en) * | 2019-05-23 | 2019-10-01 | 浙江理工大学 | A kind of preparation method handling dyeing waste water both sexes flocculation material |
| CN112375260A (en) * | 2020-11-17 | 2021-02-19 | 齐鲁工业大学 | Preparation method of glucose-based porous water-absorbing edible gel |
| CN112625306A (en) * | 2021-01-11 | 2021-04-09 | 中国制浆造纸研究院有限公司 | Full-biodegradable water-absorbent resin and preparation method thereof |
| CN114805821A (en) * | 2022-04-28 | 2022-07-29 | 上海摩漾生物科技有限公司 | Degradable antibacterial peptide based on cellulose and preparation method thereof |
| CN114805821B (en) * | 2022-04-28 | 2023-02-03 | 上海摩漾生物科技有限公司 | Degradable antibacterial peptide based on cellulose and preparation method thereof |
| CN115212349A (en) * | 2022-07-05 | 2022-10-21 | 浦易(上海)生物技术股份有限公司 | Gelable compositions, methods of preparation and uses thereof |
| CN115212349B (en) * | 2022-07-05 | 2023-11-21 | 浦易(上海)生物技术股份有限公司 | Gellable composition, method for the production and use thereof |
| CN117530929A (en) * | 2024-01-10 | 2024-02-09 | 东华大学 | Weight-losing capsule |
| CN117530929B (en) * | 2024-01-10 | 2024-03-29 | 东华大学 | Weight-losing capsule |
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