Asymmetric adhesion bionic hydrogel dressing and preparation method thereof
The asymmetric adhesion biomimetic hydrogel dressing with a double-layer structure design solves the problems of easy breakage and poor adhesion of traditional hydrogel dressings. It has self-healing and high tensile properties and is suitable for wound repair in frequently active areas.
Patent Information
- Application Number
- CN202511537805.4
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-10-27
- Publication Date
- 2026-01-20
AI Technical Summary
Traditional hydrogel dressings are prone to breakage at the wound site and lack cell affinity and tissue adhesion, especially during frequent body movements, and the problem of poor adhesion due to bilateral adhesion has not been effectively solved.
The design employs a dual-layer structure, comprising an upper double-network hydrogel and a lower mussel-like adhesive layer. The upper hydrogel is prepared by crosslinking acrylamide, acrylic acid, and N,N'-methylenebisacrylamide in FeCl3 solution, while the lower adhesive layer is prepared by a hydroxypropyl chitosan and protocatechuic acid graft copolymer, achieving a strong adhesion on one side and a low adhesion on the other.
It achieves strong adhesion to wounds and prevents poor adhesion, possesses self-healing and high tensile strength, and is suitable for wound repair in frequently moving areas.
Smart Images
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Abstract
Description
TECHNICAL FIELD
[0001] The application belongs to the technical field of biomedical materials, and relates to a hydrogel dressing for wound repair, in particular to an asymmetric adhesive biomimetic hydrogel dressing and a preparation method thereof. TECHNICAL BACKGROUND
[0002] Hydrogel is composed of a three-dimensional network structure and can contain a large amount of water to swell without dissolving. The unique properties of hydrogel have attracted the attention of many scientists, and have been developed for drug delivery, cancer treatment, bacterial infection and wound healing. Compared with other wound healing materials, hydrogel has the following advantages: 1) the high water content of hydrogel makes the wound keep a moist environment, has low adhesion to the tissue, and is easy to remove; 2) the good swelling property of hydrogel makes it have good absorption capacity, which can absorb tissue exudate; 3) the high porosity of hydrogel promotes the transmission of oxygen, which is beneficial to tissue respiration; 4) the treatment agent can be delivered to the damaged site; 5) in addition, hydrogel has a rapid self-healing ability, which can automatically repair the damage caused by movement and prolong the use time.
[0003] Traditional hydrogel has insufficient mechanical strength due to its high water content, and is easy to break at the wound site; and general super-strong hydrogel mostly lacks cell affinity and tissue adhesion, especially when the body moves frequently, which is easy to cause deformation and fall off; an ideal hydrogel auxiliary material should have strong wet tissue adhesion to avoid failure and fall off after contacting wound exudate.
[0004] With the in-depth cross-research of biomedical engineering and natural science, various biomimetic materials have been developed and used for disease treatment and management. Mussels are a common marine organism that can attach to the surface of rocks, buoys or ship bottoms for survival. In the water environment, mussels can almost adhere to the surface of any inorganic and organic materials, and from the chemical point of view, the adhesion lies in the ability of the catechol side chain of L-3,4-dihydroxyphenylalanine (L-DOPA) extracted from folded mussel foot protein (Mfp) to form different types of chemical interactions and crosslink with various substrates. Therefore, under the inspiration of mussel chemistry, components with polyphenol-like structure and amino groups can be introduced into the hydrogel dressing to endow the system with excellent adhesion performance and realize effective adhesion to the wound tissue. However, most of the current hydrogels with adhesion are bilaterally adhesive, which not only can adhere to the wound surface, but also easily adhere to the surrounding environment, causing undesirable adhesion. This problem has not been effectively solved at present. SUMMARY
[0005] The purpose of the present application is to make up for the shortcomings of the prior art, and provide an asymmetric adhesive biomimetic hydrogel dressing and a preparation method thereof; the asymmetric adhesive biomimetic hydrogel dressing comprises an upper double-network hydrogel and a lower mussel-inspired adhesive layer; the upper hydrogel is prepared from acrylamide, acrylic acid, N , N '-methylene bisacrylamide in an FeCl3 solution through a cross-linking reaction, has high mechanical strength, self-repairing performance and low adhesion; the lower adhesive layer is prepared from a hydroxypropyl chitosan and protocatechuic acid graft copolymer, and has strong adhesion. Through the double-layer structure design, one side has strong adhesion and the other side has low adhesion, which can effectively prevent undesirable adhesion, and at the same time has self-repairing, high tensile and swelling properties.
[0006] In order to achieve the above-mentioned purpose, the technical scheme adopted by the present application is as follows: The preparation method of the asymmetric adhesive biomimetic hydrogel dressing is characterized by comprising the following steps: (1) acrylamide and acrylic acid are dissolved in water according to a mass ratio of 1:9-9:1 to obtain a mixed solution; then N, N'-methylene bisacrylamide and N, N, N', N'-tetramethyl ethylenediamine in an amount of 0.1-2% of the mass of the mixed solution are added to the mixed solution, followed by adding FeCl3 in an amount of 0.3-5% of the mass of the mixed solution, and then adding persulfate amine in an amount of 0.1-2% of the mass of the mixed solution, to obtain the upper hydrogel through cross-linking; (2) protocatechuic acid in an amount of 20-50% of the mass of hydroxypropyl chitosan (mass concentration 0.2-3%), 1-(3-dimethylaminopropyl)-3-ethyl carbodiimide hydrochloride in an amount of 50-75% of the mass of hydroxypropyl chitosan (mass concentration 0.5-4.5%), and N-hydroxy succinimide in an amount of 20-50% of the mass of hydroxypropyl chitosan (mass concentration 0.2-3%) are added to a hydroxypropyl chitosan solution (mass concentration 1%-6%) to obtain the adhesive layer; (3) the adhesive layer is coated on one side of the upper hydrogel, and is cured at room temperature to obtain the asymmetric adhesive biomimetic hydrogel dressing.
[0007] Further, the asymmetric adhesive biomimetic hydrogel dressing comprises an upper double-network hydrogel and a lower mussel-inspired adhesive layer; the upper hydrogel is prepared from acrylamide, acrylic acid, N , N '-methylene bisacrylamide in an FeCl3 solution through a cross-linking reaction, and the lower adhesive layer is prepared from a hydroxypropyl chitosan and protocatechuic acid graft copolymer.
[0008] In view of the respective advantages of adhesive tape and hydrogel as wound dressings, the present application designs an asymmetric adhesive hydrogel dressing in the form of "glue tape"; acrylamide, acrylic acid,N , N Methylene bisacrylamide in FeCl3 solution, with persulfate amine as initiator to prepare a double crosslinking network hydrogel as the upper layer of the adhesive layer, to graft copolymerize a certain concentration of hydroxypropyl chitosan and protocatechuic acid under the action of EDC / NHS, to obtain an adhesive layer; coat the adhesive layer on one side of the upper layer hydrogel, and solidify at room temperature to obtain an asymmetric adhesive biomimetic hydrogel dressing.
[0009] Compared with the prior art, the asymmetric adhesive biomimetic hydrogel dressing has the following advantages: 1. The preparation process of the asymmetric adhesive biomimetic hydrogel dressing is simple and easy to operate, and is conducive to large-scale industrial production. 2. A multifunctional hydrogel dressing with mechanical properties and adhesive properties and a research method thereof are obtained. 3. The asymmetric adhesive biomimetic hydrogel dressing prepared has one side with good adhesive properties and the other side with low adhesive properties. Therefore, such a double-sided hydrogel can be firmly adhered to the tissue and can prevent the generation of undesirable adhesion. BRIEF DESCRIPTION OF DRAWINGS
[0010] Figure 1 It is a product photo of an asymmetric adhesive biomimetic hydrogel dressing; Figure 2 It is a skin adhesion effect diagram of an asymmetric adhesive biomimetic hydrogel dressing product; Figure 3 It is a pig skin stretching diagram of an asymmetric adhesive biomimetic hydrogel dressing product; Figure 4 It is a pig skin tensile stress-strain curve diagram of an asymmetric adhesive biomimetic hydrogel dressing product; Figure 5 It is a tensile strain capacity curve diagram of an asymmetric adhesive biomimetic hydrogel dressing prepared at different Fe3+ concentrations. DETAILED DESCRIPTION
[0011] A preparation method of an asymmetric adhesive biomimetic hydrogel dressing, the specific implementation steps are as follows: Example 1
[0012] (1) Dissolve 1.2 g of acrylamide and 1.12 mL of acrylic acid in 10 mL of water, add 20 mg of N, N'-methylene bisacrylamide and 20 μL of N , N , N ', N - tetramethyl ethylenediamine, add 0.0135 g of FeCl3, and then add 20 mg of persulfate amine to the solution, and crosslink for 24 hours to obtain an upper layer hydrogel; (2) To 10 mL of 4% hydroxypropyl chitosan solution, 0.2 g of protocatechuic acid, 0.48 g of 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and 0.29 g of N-hydroxysuccinimide were added to obtain an adhesion layer; (3) The adhesion layer was coated on one side of the upper hydrogel, and cured at room temperature to obtain an asymmetric adhesion biomimetic hydrogel dressing. Example 2
[0013] (1) 1.2 g of acrylamide and 0.5 mL of acrylic acid were dissolved in 10 mL of water, 40 mg of N, N'-methylenebisacrylamide and 40 μL of N , N , N ', N - tetramethyl ethylenediamine were added, 0.003 g of FeCl 3， Then 40 mg of ammonium persulfate was added to the solution, and cross-linked for 6 hours to obtain the upper hydrogel; (2) To 10 mL of 2% hydroxypropyl chitosan solution, 0.2 g of protocatechuic acid, 0.48 g of 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and 0.29 g of N-hydroxysuccinimide were added to obtain an adhesion layer; (3) The adhesion layer was coated on one side of the upper hydrogel, and cured at room temperature to obtain an asymmetric adhesion biomimetic hydrogel dressing. Example 3
[0014] (1) 1.2 g of acrylamide and 2.72 mL of acrylic acid were dissolved in 10 mL of water, 80 mg of N, N'-methylenebisacrylamide and 80 μL of N , N , N ', N - tetramethyl ethylenediamine were added, 0.5 g of FeCl 3， Then 80 mg of ammonium persulfate was added to the solution, and cross-linked for 12 hours to obtain the upper hydrogel; (2) To 10 mL of 6% hydroxypropyl chitosan solution, 0.2 g of protocatechuic acid, 0.48 g of 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and 0.29 g of N-hydroxysuccinimide were added to obtain an adhesion layer; (3) The adhesion layer was coated on one side of the upper hydrogel, and cured at room temperature to obtain an asymmetric adhesion biomimetic hydrogel dressing.
[0015] The asymmetric adhesion biomimetic hydrogel dressing prepared by the application is suitable for repairing various wounds, and is especially suitable for wound care of frequently moving parts.
[0016] Finally, it should be noted that the above examples are intended to be illustrative only and not limiting of the technical solutions of the present application. Any equivalent replacements, modifications or partial replacements of the present application that do not depart from the spirit and scope of the present application shall be covered within the scope of protection of the claims of the present application.
Claims
1. A method of preparing an asymmetric adhesive biomimetic hydrogel dressing, characterized by The method comprises the following steps: (1) dissolving acrylamide and acrylic acid in water at a mass ratio of 1:9-9:1 to obtain a mixed solution; then adding 0.1-2% of N, N'-methylenebisacrylamide and 0.1-2% of N, N, N', N'-tetramethyl ethylenediamine by mass of the mixed solution into the mixed solution, and then adding 0.3-5% of FeCl3 by mass of the mixed solution into the mixed solution, and then adding 0.1-2% of ammonium persulfate by mass of the mixed solution into the solution, and then cross-linking to obtain an upper hydrogel; (2) adding 20-50% of protocatechuic acid, 50-75% of 1-(3-dimethylaminopropyl)-3-ethyl carbodiimide hydrochloride and 20-50% of N-hydroxysuccinimide by mass of hydroxypropyl chitosan into a hydroxypropyl chitosan solution to obtain an adhesion layer; (3) coating the adhesion layer on one side of the upper hydrogel, and curing at room temperature to obtain an asymmetric adhesion biomimetic hydrogel dressing.
2. The process for the preparation of asymmetric adhesive biomimetic hydrogel dressing as claimed in claim 1, wherein: The mass concentration of the hydroxypropyl chitosan solution in step (2) is 1%-6%.
3. The process for the preparation of asymmetric adhesive biomimetic hydrogel dressing as claimed in claim 1, wherein: The mass concentration of the protocatechuic acid in step (2) is 0.2-3%.
4. The process for the preparation of asymmetric adhesive biomimetic hydrogel dressing as claimed in claim 1, wherein: The mass concentration of the 1-(3-dimethylaminopropyl)-3-ethyl carbodiimide hydrochloride in step (2) is 0.5-4.5%.
5. The process for the preparation of asymmetric adhesive biomimetic hydrogel dressing as claimed in claim 1, wherein: The mass concentration of the N-hydroxysuccinimide in step (2) is 0.2-3%.
6. An asymmetric adhesive biomimetic hydrogel dressing prepared according to the method of any one of claims 1 to 5, characterized in that: The asymmetric adhesion biomimetic hydrogel dressing comprises an upper double-network hydrogel and a lower mussel-inspired adhesion layer.