CN113754830A - Hydrogel with wet-state adhesion performance and preparation method and application thereof - Google Patents
Hydrogel with wet-state adhesion performance and preparation method and application thereof Download PDFInfo
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- CN113754830A CN113754830A CN202110909626.4A CN202110909626A CN113754830A CN 113754830 A CN113754830 A CN 113754830A CN 202110909626 A CN202110909626 A CN 202110909626A CN 113754830 A CN113754830 A CN 113754830A
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F251/00—Macromolecular compounds obtained by polymerising monomers on to polysaccharides or derivatives thereof
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F2/00—Processes of polymerisation
- C08F2/44—Polymerisation in the presence of compounding ingredients, e.g. plasticisers, dyestuffs, fillers
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
- C09J11/02—Non-macromolecular additives
- C09J11/06—Non-macromolecular additives organic
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J151/00—Adhesives based on graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Adhesives based on derivatives of such polymers
- C09J151/02—Adhesives based on graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Adhesives based on derivatives of such polymers grafted on to polysaccharides
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Abstract
The invention discloses a hydrogel with wet-state adhesion performance, and a preparation method and application thereof. The hydrogel with wet adhesion performance is prepared from the following raw materials in parts by mass: acrylic acid: 100 parts of (A); quaternized xylan: 10-30 parts; tannic acid: 3-6 parts; a crosslinking agent: 0.1 to 1 portion; initiator: 0.1 to 1 portion; water: 150 to 400 portions. The hydrogel disclosed by the invention has excellent mechanical properties and underwater adhesion properties, is environment-friendly, has a simple preparation method, and is easy to realize industrial large-scale production.
Description
Technical Field
The invention relates to the technical field of hydrogel materials, in particular to hydrogel with wet-state adhesion performance and a preparation method and application thereof.
Background
The hydrogel is a material with a three-dimensional network structure generated by hydrophilic macromolecules through physical action or chemical reaction, has certain fluidity on the premise of keeping mechanical property, and has a structure similar to a natural extracellular matrix, so that the hydrogel has a good application prospect in the fields of wearable biosensors, biological adhesives, medical dressings and the like. However, hydrogels absorb water easily, and form a water film between the hydrogel and the substrate, which greatly reduces the adhesion property of the hydrogel to the substrate, especially under wet conditions and in water environment, and conventional hydrogels often lose the adhesion property completely, which greatly limits the application of the hydrogel.
In recent years, researchers have conducted extensive studies on the wet adhesion of hydrogels, and developed some hydrogels that can be used in a wet environment, but these hydrogels still have significant drawbacks or shortcomings, mainly expressed in the following aspects: 1) the adhesion force of the hydrogel in a wet environment is still weak, and the adhesion strength is not enough; 2) has certain toxicity, is not safe enough and is environment-friendly; 3) hydrogels are susceptible to significant swelling and ultimately deformation.
Therefore, it is of great importance to develop a hydrogel having excellent wet adhesion properties.
Disclosure of Invention
The invention aims to provide a hydrogel with wet-state adhesion performance, and a preparation method and application thereof.
The technical scheme adopted by the invention is as follows:
a hydrogel with wet adhesion performance is prepared from the following raw materials in parts by mass:
acrylic acid: 100 parts of (A);
quaternized xylan: 10-30 parts;
tannic acid: 3-6 parts;
a crosslinking agent: 0.1 to 1 portion;
initiator: 0.1 to 1 portion;
water: 150 to 400 portions.
Preferably, the quaternized xylan is prepared by the following method: firstly, alkalizing and modifying xylan, and then reacting with 2, 3-epoxypropyl trimethyl ammonium chloride to obtain the quaternized xylan.
Further preferably, the quaternized xylan is prepared by the following method: dispersing xylan in water, adding sodium hydroxide or/and potassium hydroxide, performing alkalization modification for 20-40 min, adding 2, 3-epoxypropyl trimethyl ammonium chloride, and performing microwave reaction at 60-80 ℃ for 20-45 min to obtain quaternized xylan.
Still further preferably, the quaternized xylan is prepared by the following method: dispersing xylan in water to prepare a xylan solution with the concentration of 3-5 wt%, adding sodium hydroxide or/and potassium hydroxide in water to prepare an alkali solution, adding the alkali solution into the xylan solution, performing alkalization modification for 20-40 min, adding 2, 3-epoxypropyltrimethylammonium chloride, performing microwave reaction at 60-80 ℃ for 20-45 min, cooling to room temperature, adding absolute ethyl alcohol to precipitate a product, washing the precipitate with an ethanol solution, dissolving with water, dialyzing for 5-10 days, and performing freeze drying to obtain the quaternized xylan.
Preferably, the molar ratio of xylose units in the xylan to sodium hydroxide or/and potassium hydroxide is 1: 0.8-1: 1.2.
Preferably, the molar ratio of the xylose units in the xylan to the 2, 3-epoxypropyltrimethylammonium chloride is 1: 5.0-1: 6.5.
Preferably, the cross-linking agent is a bisacrylamide cross-linking agent.
Further preferably, the cross-linking agent is N, N' -methylenebisacrylamide.
Preferably, the initiator is a persulfate initiator.
Further preferably, the initiator is at least one of ammonium persulfate, potassium persulfate and sodium persulfate.
The preparation method of the hydrogel with wet-state adhesive property comprises the following steps: dispersing acrylic acid in water, adding quaternized xylan, tannic acid and a crosslinking agent for mixing, adding an initiator for mixing, pouring the obtained mixed solution into a mould for crosslinking reaction, and obtaining the hydrogel with wet-state adhesion performance.
Preferably, the crosslinking reaction is carried out at 50 ℃ to 70 ℃.
Preferably, the time of the crosslinking reaction is 4 to 8 hours.
The invention has the beneficial effects that: the hydrogel disclosed by the invention has excellent mechanical properties and underwater adhesion properties, is environment-friendly, has a simple preparation method, and is easy to realize industrial large-scale production.
Specifically, the method comprises the following steps:
1) the invention adopts xylan and tannic acid from biomass to prepare hydrogel with adhesiveness under wet condition, the adhesion performance of the hydrogel in air and the adhesion performance under water are realized by introducing the polyphenol structure of the tannic acid and other substances to form hydrogen bond action, pi-pi action, electrostatic action, covalent bond action and the like, quaternized xylan is grafted with acrylic acid to construct a hydrogel network structure, and positive charge is introduced to form a network structure in the hydrogel through electrostatic action, the adhesion effect on a substrate is realized through electrostatic action, the introduction of the acrylic acid can form the network structure of the hydrogel on one hand, and on the other hand, the problem that the quaternized xylan and the tannic acid are easy to precipitate in aqueous solution is solved;
2) the xylan adopted by the invention is derived from biomass, the xylan has the performances of biocompatibility, degradability and the like, and the modified quaternized xylan has cationic property, water solubility and special physical and chemical properties and is a good material for preparing hydrogel;
3) the tannic acid adopted by the invention is derived from biomass, has a polyphenol structure, and has various physical and chemical properties (such as: antibacterial property, oxidation resistance and the like), the abundant polyphenol groups can generate hydrogen bonds and other functional groups to form hydrogel, and in addition, the structure can endow the hydrogel with excellent adhesion performance;
4) the acrylic acid adopted by the invention can play a role in enhancing the strength of the xylan-based hydrogel, and the quaternized xylan and the tannic acid can be dispersed in the aqueous solution simultaneously without flocculation;
5) the invention expands the application of xylan hemicellulose and provides an effective way for high-value utilization of the hemicellulose.
Drawings
FIG. 1 is a graph showing the effect of acrylic acid on the dispersion of quaternized xylan and tannin precipitates.
FIG. 2 is a graph showing the adhesion effect of the hydrogel having wet adhesion properties of example 1 on different substrates under water.
FIG. 3 is a graph showing the results of the shear strength test of the hydrogel having wet adhesion properties of example 2 for different materials of the substrate in air and under water.
FIG. 4 is a graph showing the results of the test of the adhesion strength of the hydrogel having wet adhesion properties of examples 1 to 3 to an aluminum plate in air.
FIG. 5 is a graph showing the results of tensile strength tests of the hydrogels having wet adhesion properties of examples 1 to 3.
FIG. 6 is a diagram of the signal of the hydrogel with wet adhesion property of example 3 for sensing finger bending underwater.
Detailed Description
The invention will be further explained and illustrated with reference to specific examples.
The quaternized xylan of examples 1 to 3 was prepared by the following method: dispersing xylan in water to prepare a xylan solution with the concentration of 5 wt%, adding sodium hydroxide into water to prepare a sodium hydroxide solution, adding the sodium hydroxide solution into the xylan solution, adding the xylan solution into the xylan solution, wherein the molar ratio of xylose units in xylan to sodium hydroxide is 1:1, performing alkalization modification for 30min, adding 2, 3-epoxypropyltrimethylammonium chloride, wherein the molar ratio of xylose units in xylan to 2, 3-epoxypropyltrimethylammonium chloride is 1:5.5, placing the reaction solution into a microwave reactor, controlling the power of the microwave reactor to be 400W, heating to 70 ℃, reacting for 35min, cooling to room temperature, adding absolute ethyl alcohol to precipitate a product, washing and precipitating with an ethanol solution with the concentration of 80 wt%, dissolving with water, dialyzing for 7 days, and performing freeze drying to obtain the quaternized xylan.
Example 1:
a hydrogel having wet adhesion properties, prepared by a process comprising the steps of:
dispersing 100g of acrylic acid in 400mL of deionized water, adding 10g of quaternized xylan, 4.5g of tannic acid and 0.2g of N, N' -methylene bisacrylamide, uniformly stirring, adding 0.5g of ammonium persulfate, uniformly stirring, pouring the obtained mixed solution into a mold, and crosslinking at 55 ℃ for 4 hours to obtain the hydrogel with wet-state adhesive property.
Example 2:
a hydrogel having wet adhesion properties, prepared by a process comprising the steps of:
dispersing 100g of acrylic acid in 230mL of deionized water, adding 20g of quaternized xylan, 5g of tannic acid and 0.3g of N, N' -methylene bisacrylamide, uniformly stirring, adding 0.6g of ammonium persulfate, uniformly stirring, pouring the obtained mixed solution into a mold, and crosslinking at 60 ℃ for 6 hours to obtain the hydrogel with wet-state adhesive property.
Example 3:
a hydrogel having wet adhesion properties, prepared by a process comprising the steps of:
dispersing 100g of acrylic acid in 150mL of deionized water, adding 30g of quaternized xylan, 5.5g of tannic acid and 0.4g of N, N' -methylene bisacrylamide, uniformly stirring, adding 0.8g of ammonium persulfate, uniformly stirring, pouring the obtained mixed solution into a mold, and crosslinking for 7 hours at 70 ℃ to obtain the hydrogel with wet-state adhesive property.
And (3) performance testing:
1) the dispersion effect of the resulting acrylic acid on the quaternized xylan and tannin precipitate was tested by dispersing 10g of quaternized xylan in 400mL of water, adding 4.5g of tannic acid, and then 100g of acrylic acid, as shown in FIG. 1.
As can be seen from fig. 1: the flocculation can occur when tannic acid is directly added into the quaternized xylan dispersion, but the flocculation disappears after acrylic acid is continuously added, so that the problem that the quaternized xylan and tannic acid can precipitate in the coexistence of aqueous solution is solved by the introduction of acrylic acid.
2) The hydrogel having wet adhesion property of example 1 was cut into a sheet having a size of 2cm × 2cm × 0.2cm, one side of the hydrogel was attached to a weight, and the other side was attached to the surface of a substrate (glass, polypropylene plastic cover, polytetrafluoroethylene, rubber, and aluminum plate) of various materials placed under water, and after contacting for 30 seconds, the adhesion effect was observed, and a graph of the adhesion effect of the hydrogel having wet adhesion property of example 1 obtained by testing under water for different materials of substrates is shown in fig. 2. Further, after contacting for 30 seconds, the weight was moved up and down and left and right in the water, and no substrate was observed to be peeled off.
As can be seen from fig. 2: the hydrogel with wet adhesion performance in example 1 has good adhesion effect under water for different base materials.
3) The hydrogel having wet adhesion properties of example 2 was cut into a sheet having a size of 2cm × 2cm × 0.1cm, placed between two substrates having the same size (made of glass, polypropylene plastic, polytetrafluoroethylene, and aluminum, respectively), applied with a certain pressure for 2min, and then placed in air or under water for a certain time, and then the two substrates were vertically and parallelly stretched at a speed of 50mm/min on a universal material testing machine until the hydrogel was separated from the substrates, and the adhesion strength was measured, which is a value of the maximum tensile force to the adhesion area ratio, and the results of the test of the shear strength of the hydrogel having wet adhesion properties of example 2 in air and under water for different materials of the substrates were shown in fig. 3.
As can be seen from fig. 3: the hydrogel with wet adhesion property of example 2 has good adhesion property in air and under water for different material substrates.
4) The hydrogel having wet adhesion properties of examples 1 to 3 was tested for adhesion strength (i.e., shear strength) to an aluminum plate in air according to the test method of reference 3), and the test results are shown in fig. 4.
As can be seen from fig. 4: the hydrogel with the wet adhesion property of examples 1-3 has good adhesion property to an aluminum plate in air, and the hydrogel with the wet adhesion property of example 1 has the best adhesion property.
5) The test results of tensile strength of the hydrogels having wet adhesion properties of examples 1 to 3 obtained by cutting the hydrogels having wet adhesion properties of examples 1 to 3 into sheets having a size of 2cm × 2cm × 0.1cm, clamping the cut hydrogels in a jig of a universal testing machine having a distance of 5mm, stretching the hydrogels at a speed of 100mm/min until the hydrogel is broken, recording the tensile stress at the time of breaking the hydrogels, and testing the obtained hydrogels having wet adhesion properties of examples 1 to 3 are shown in fig. 5.
As can be seen from fig. 5: the hydrogels of examples 1-3 with wet adhesion all had good mechanical properties.
6) The hydrogel with wet adhesion property of example 3 was directly adhered and fixed on a finger, a loop was formed by two silver wires and a universal digital meter, the finger was placed under water and repeatedly bent at 90 degrees, the resistance change was recorded, and the signal graph of the hydrogel with wet adhesion property of example 3 obtained by testing under water for sensing finger bending is shown in fig. 6.
As can be seen from fig. 6: the hydrogel having wet adhesion properties of example 3 is able to generate a good signal of finger bending under water, and thus monitoring of motion can be achieved.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.
Claims (10)
1. The hydrogel with wet adhesion performance is characterized by being prepared from the following raw materials in parts by mass:
acrylic acid: 100 parts of (A);
quaternized xylan: 10-30 parts;
tannic acid: 3-6 parts;
a crosslinking agent: 0.1 to 1 portion;
initiator: 0.1 to 1 portion;
water: 150 to 400 portions.
2. The hydrogel having wet adhesion properties of claim 1, wherein: the quaternized xylan is prepared by the following method: firstly, alkalizing and modifying xylan, and then reacting with 2, 3-epoxypropyl trimethyl ammonium chloride to obtain the quaternized xylan.
3. The hydrogel having wet adhesion properties of claim 2, wherein: the quaternized xylan is prepared by the following method: dispersing xylan in water, adding sodium hydroxide or/and potassium hydroxide, performing alkalization modification for 20-40 min, adding 2, 3-epoxypropyl trimethyl ammonium chloride, and performing microwave reaction at 60-80 ℃ for 20-45 min to obtain quaternized xylan.
4. The hydrogel having wet adhesion properties of claim 3, wherein: the molar ratio of xylose units in the xylan to sodium hydroxide or/and potassium hydroxide is 1: 0.8-1: 1.2; the molar ratio of xylose units in the xylan to 2, 3-epoxypropyltrimethylammonium chloride is 1: 5.0-1: 6.5.
5. The hydrogel having wet adhesion properties according to any one of claims 1 to 4, wherein: the cross-linking agent is a bisacrylamide cross-linking agent.
6. The hydrogel having wet adhesion properties according to any one of claims 1 to 4, wherein: the initiator is a persulfate initiator.
7. The method for preparing the hydrogel having wet adhesion properties according to any one of claims 1 to 6, comprising the steps of: dispersing acrylic acid in water, adding quaternized xylan, tannic acid and a crosslinking agent for mixing, adding an initiator for mixing, pouring the obtained mixed solution into a mould for crosslinking reaction, and obtaining the hydrogel with wet-state adhesion performance.
8. The method for preparing a hydrogel having wet adhesion properties according to claim 7, wherein: the crosslinking reaction is carried out at 50-70 ℃.
9. The method for producing a hydrogel having wet adhesion properties according to claim 7 or 8, wherein: the time of the cross-linking reaction is 4-8 h.
10. Use of the hydrogel having wet adhesion properties according to any one of claims 1 to 6 for adhesion in air or water.
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Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114404646A (en) * | 2021-12-28 | 2022-04-29 | 安徽大学 | CM-beta-CD supported tannic acid polyacrylamide type double-network antibacterial hydrogel |
CN114891157A (en) * | 2022-05-17 | 2022-08-12 | 华南理工大学 | Rapid adhesion wood-based gel and preparation method and application thereof |
CN115558439A (en) * | 2022-10-11 | 2023-01-03 | 广西至善新材料科技有限公司 | Modified xylan adhesive and preparation method and application thereof |
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CN107353559A (en) * | 2017-06-23 | 2017-11-17 | 华南理工大学 | A kind of high intensity magnetic coupling hydrogel of quaternized xylan/nano-cellulose enhancing and preparation method and application |
CN109331216A (en) * | 2018-11-28 | 2019-02-15 | 福建师范大学 | A kind of quick-acting haemostatic powder hydrogel and preparation method thereof |
CN111514367A (en) * | 2020-04-29 | 2020-08-11 | 北京大学 | Wound adhesive hydrogel material, preparation method and application thereof |
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2021
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US20030232895A1 (en) * | 2002-04-22 | 2003-12-18 | Hossein Omidian | Hydrogels having enhanced elasticity and mechanical strength properties |
CN107353559A (en) * | 2017-06-23 | 2017-11-17 | 华南理工大学 | A kind of high intensity magnetic coupling hydrogel of quaternized xylan/nano-cellulose enhancing and preparation method and application |
CN109331216A (en) * | 2018-11-28 | 2019-02-15 | 福建师范大学 | A kind of quick-acting haemostatic powder hydrogel and preparation method thereof |
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Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114404646A (en) * | 2021-12-28 | 2022-04-29 | 安徽大学 | CM-beta-CD supported tannic acid polyacrylamide type double-network antibacterial hydrogel |
CN114891157A (en) * | 2022-05-17 | 2022-08-12 | 华南理工大学 | Rapid adhesion wood-based gel and preparation method and application thereof |
CN114891157B (en) * | 2022-05-17 | 2023-03-24 | 华南理工大学 | Rapid adhesion wood-based gel and preparation method and application thereof |
CN115558439A (en) * | 2022-10-11 | 2023-01-03 | 广西至善新材料科技有限公司 | Modified xylan adhesive and preparation method and application thereof |
CN115558439B (en) * | 2022-10-11 | 2023-10-24 | 广西至善新材料科技有限公司 | Modified xylan adhesive and preparation method and application thereof |
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