Self-repairing conductive hydrogel material based on dynamic acylhydrazone bond and hydrogen bond as well as preparation method and application of self-repairing conductive hydrogel material

By introducing dynamic acylhydrazone bonds and hydrogen bonds into conductive hydrogels, combined with acrylamide and carbon-based conductive fillers, a hydrogel material with efficient self-healing and stable conductive properties was successfully prepared, solving the problems faced by existing conductive hydrogels. Problems of structural damage and electrical performance degradation under the action of external forces.

CN119331172AActive Publication Date: 2025-01-21SHAANXI UNIV OF SCI & TECH

Patent Information

Application Number
CN202411505919.6
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2024-10-28
Publication Date
2025-01-21
Estimated Expiration
2044-10-28

AI Technical Summary

Technical Problem

When existing conductive hydrogels are extruded by external forces, microscopic cracks will occur on the surface of the material, which will affect structural integrity and electrical properties, and will be difficult to self-repair, resulting in a shortening of the material life.

Method used

A self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds is used to modify natural polysaccharides through oxidants and hydrazide modifiers to form reversible acylhydrazone bonds and hydrogen bonds, combining acrylamide, hydrophobic monomers and Carbon-based conductive fillers have successfully prepared hydrogel materials with stable conductive properties and excellent self-healing properties through free radical polymerization.

Benefits of technology

It achieves the mechanical properties of high ionic conductivity and high breaking tensile, has good self-healing performance, high sensitivity and stable electrical properties, and is suitable for fields such as flexible sensors.

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Abstract

The invention discloses preparation and application of a self-repairing conductive hydrogel material based on a dynamic acylhydrazone bond and a hydrogen bond, and belongs to the field of flexible electronic materials.The preparation method comprises the steps that acrylamide serves as a monomer, a carbon-based material serves as a conductive filler, a hydrophobic monomer is combined, and a polymer network framework is prepared through a free radical polymerization method; the preparation method comprises the following steps: preparing natural polysaccharide, modifying and grafting the natural polysaccharide by adopting an oxidizing agent and a hydrazide modifier to obtain aldehyde polysaccharide and hydrazide polysaccharide, and introducing the aldehyde polysaccharide and the hydrazide polysaccharide into a polymer network skeleton to prepare the self-repairing conductive hydrogel based on a dynamic acylhydrazone bond and hydrogen bond network structure. The prepared self-repairing conductive hydrogel not only has the mechanical properties of high ionic conductivity and high fracture tensile strength, but also has the characteristics of good repairability, high sensitivity, stable electrical property and the like; the method is easy to operate, simple in step and suitable for a plurality of related fields such as wearable electronic equipment, flexible strain sensors and electronic skin.
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Description

Technical Field

[0001] The present invention belongs to the technical field of functional materials and relates to flexible electronic materials, and in particular to a self-repairing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, and a preparation method and application thereof. Background Art

[0002] As a polymer material with a three-dimensional network cross-linked structure, hydrogel has become an important material in the fields of energy, agriculture, and materials science due to its high water content and excellent biocompatibility and mechanical properties. By adding conductive fillers such as conductive polymers, carbon-based materials, metal salts, and ionic liquids to the hydrogel matrix, the hydrogel is endowed with conductive properties, which shows great application potential in many fields such as flexible sensor technology, biomedical engineering, and smart materials.

[0003] At present, the research results of conductive hydrogels are remarkable, but they still face some challenges. When conductive hydrogels are squeezed by external forces, microscopic cracks will appear on the surface of the material, which will affect the integrity and electrical properties of the hydrogel structure, thereby greatly shortening the life of the material, and the damaged hydrogel is difficult to repair by artificial methods. Self-repairing hydrogels can spontaneously repair damage or repair through the intervention of external stimuli (such as pH, light, temperature), so the self-repair process can be divided into spontaneous and non-spontaneous. Among them, non-spontaneous self-repairing materials are microcapsules, nanocontainers or microvascular systems containing monomers, crosslinkers or catalysts placed inside the gel material. When damage occurs, these repair agents will be released into the gel matrix, thereby inducing in situ polymerization to repair the damage of the hydrogel. However, this method is difficult to prepare hydrogels, and the repair agent can only be implanted once or self-repair can only be performed once, which greatly limits the service life of the material. Therefore, efficient and spontaneously repairable conductive hydrogel materials have become a research hotspot. Summary of the invention

[0004] In view of the shortcomings of the prior art, the purpose of the present invention is to provide a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, and a preparation method and application thereof, which has mechanical properties of high ionic conductivity and high tensile strength at break, excellent self-healing and conductive stability, and is applied to flexible sensors with high sensitivity, high ionic conductivity and high tensile strength at break.

[0005] In order to achieve the above object, the present invention adopts the following technical solutions:

[0006] A method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds comprises the following steps:

[0007] Step 1, dissolving 2 to 8 parts of natural polysaccharide in 70 to 90 parts of deionized water by mass, adding 4 to 6 parts of oxidant, stirring at 30 to 50° C. for 2 to 4 hours, separating the solid, washing, and drying to obtain the aldehyde-modified polysaccharide; dissolving 2 to 8 parts of natural polysaccharide in 70 to 90 parts of deionized water, adding 0.3 to 0.5 parts of hydrazide modifier, stirring at 35 to 45° C. for 2 to 3 hours, separating the solid, washing, and drying to obtain the hydrazide-modified polysaccharide;

[0008] Step 2: Dissolve 2 to 6 parts of carbon-based material in 70 to 90 parts of deionized water by mass, add 4 to 6 parts of reducing agent, stir and react at 40 to 50° C. for 1 to 2 hours, separate the solid, wash and dry to obtain a conductive filler;

[0009] Step three, dissolve 3 to 8 parts of acrylamide in 70 to 90 parts of deionized water by mass, stir and dissolve at 50 to 60°C, then add 2 to 4 parts of hydrophobic monomer, 0.06 to 0.08 parts of cross-linking agent MBA and 2 to 5 parts of aldehyde-modified polysaccharide prepared in step one, 1 to 6 parts of hydrazide-modified polysaccharide prepared in step one and 2 to 5 parts of conductive filler prepared in step two, react at 50 to 60°C with N2 for 1 to 3 hours, add 0.1 to 0.5 parts of initiator dropwise, and react at 60 to 70°C for 1 to 2 hours to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

[0010] The present invention also has the following technical features:

[0011] Preferably, the natural polysaccharide includes any one of pectin, guar gum, starch, agar and lignin.

[0012] Preferably, the oxidant includes any one of sodium periodate, sodium hypochlorite, hydrogen peroxide and ferric oxychloride.

[0013] Preferably, the hydrazide modifier includes any one of adipic acid dihydrazide, succinic acid dihydrazide, maleic acid dihydrazide and p-nitrobenzoic acid hydrazide.

[0014] Preferably, the carbon-based material includes any one of graphene, graphene oxide, silicon carbide fiber, carbon powder and multi-walled carbon nanotubes.

[0015] Preferably, the reducing agent includes any one of polydopamine, sodium sulfite and L-cysteine.

[0016] Preferably, the hydrophobic monomer includes any one of octadecyl methacrylate, isooctyl acrylate, isobutyl acrylate, isodecyl acrylate, isobutyl methacrylate and octyl methacrylate.

[0017] Preferably, the initiator comprises one of sodium persulfate, ammonium persulfate and potassium persulfate.

[0018] The present invention also protects a self-repairing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds prepared by the method as described above, and its application in a flexible strain sensor.

[0019] Compared with the prior art, the present invention has the following technical effects:

[0020] The present invention uses acrylamide, hydrophobic monomers, natural polysaccharides, carbon-based conductive fillers and the like as main raw materials. Natural polysaccharides have good biodegradability and biocompatibility, are non-toxic, and have good adsorption and moisture retention properties. The natural polysaccharides are modified by an oxidant and a hydrazide modifier to obtain aldehyde-modified polysaccharides and hydrazide-modified polysaccharides, wherein the aldehyde group and the hydrazide group react to form a reversible dynamic acylhydrazone bond. Then, acrylamide, hydrophobic monomers, and carbon-based conductive fillers are introduced, and a hydrogel material with stable conductive properties and excellent self-healing properties is successfully prepared by free radical polymerization. The introduction of reversible dynamic acylhydrazone bonds and hydrogen bonds in the hydrogel gives the hydrogel excellent self-healing properties. The prepared self-healing conductive hydrogel not only has high ionic conductivity and high tensile strength at break mechanical properties, but also has the characteristics of good repairability, high sensitivity, stable electrical properties, and the like.

[0021] The invention is simple to operate and has concise steps. It is applicable to multiple related fields such as wearable electronic devices, flexible strain sensors, and electronic skin. When applied to flexible strain sensors, the sensors have excellent sensitivity, high ionic conductivity, and high breaking elongation, providing a new solution for the development of flexible electronic devices.

[0022] The biocompatibility and self-healing properties of the present invention provide new possibilities for application in flexible electronic devices, biomedical engineering and other fields, and are expected to become an important component of future flexible electronic devices and biomedical engineering. BRIEF DESCRIPTION OF THE DRAWINGS

[0023] Figure 1 This is a self-repairing effect diagram of Example 1 of the present invention;

[0024] Figure 2 This is a diagram showing the conductive effect of Example 1 of the present invention;

[0025] Figure 3 It is a reaction mechanism diagram of Example 1 of the present invention. DETAILED DESCRIPTION

[0026] The specific contents of the present invention are further explained in detail below in conjunction with embodiments.

[0027] Example 1

[0028] This embodiment provides a method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, comprising the following steps. The reaction mechanism is as follows: Figure 3As shown:

[0029] Step 1, dissolving 5 parts of pectin in 70 parts of deionized water by mass, adding 4 parts of sodium periodate and stirring at 40° C. for 4 hours, filtering, washing and drying to obtain aldehyde-modified pectin; dissolving 5 parts of pectin in 70 parts of deionized water, adding 0.3 parts of adipic acid dihydrazide and stirring at 40° C. for 3 hours, centrifuging or filtering, washing and purifying with water and ethanol, and then freeze-drying to obtain hydrazide-modified pectin;

[0030] Step 2, dissolving 3 parts of graphene oxide in 70 parts of deionized water by mass, adding 4 parts of polydopamine, stirring and reacting at 45° C. for 2 hours, centrifuging or filtering, washing with water and ethanol for purification, and freeze-drying to obtain a conductive filler;

[0031] Step 3: Dissolve 4 parts of acrylamide in 70 parts of deionized water by mass, stir and dissolve at 60°C, then add 2 parts of octadecyl methacrylate, 0.06 parts of crosslinker MBA, 2 parts of formaldehyde-modified pectin, 1 part of hydrazide-modified pectin and 2 parts of conductive fillers, react at 60°C with N2 for 1 hour, add 0.1 parts of initiator ammonium persulfate dropwise, and react at 70°C for 2 hours to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

[0032] Example 2

[0033] This embodiment provides a method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, comprising the following steps:

[0034] Step 1, dissolving 5 parts of starch in 80 parts of deionized water by mass, adding 5 parts of sodium periodate and stirring at 30° C. for 2 hours, filtering, washing and drying to obtain aldehyde-modified starch; dissolving 5 parts of starch in 80 parts of deionized water, adding 0.4 parts of succinic acid dihydrazide and stirring at 35° C. for 2 hours, centrifuging or filtering, washing and purifying with water and ethanol, and then freeze-drying to obtain hydrazide-modified starch;

[0035] Step 2, dissolving 4 parts of carbon powder in 80 parts of deionized water by mass, adding 5 parts of sodium sulfite and stirring at 40° C. for 1 hour, centrifuging or filtering, washing with water and ethanol for purification, and freeze-drying to obtain a conductive filler;

[0036] Step 3: Dissolve 5 parts of acrylamide in 80 parts of deionized water by mass, stir and dissolve at 60°C, then add 3 parts of isooctyl acrylate, 0.07 parts of crosslinker MBA, 3 parts of formaldehyde-modified starch, 2 parts of hydrazide-modified starch and 3 parts of conductive filler, react at 50°C with N2 for 3 hours, add 0.2 parts of initiator ammonium persulfate dropwise, and react at 60°C for 1 hour to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

[0037] Example 3

[0038] This embodiment provides a method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, comprising the following steps:

[0039] Step 1, dissolving 6 parts of agar in 90 parts of deionized water by mass, adding 6 parts of hydrogen peroxide and stirring at 50° C. for 3 hours, filtering, washing and drying to obtain aldehyde-modified agar; dissolving 6 parts of agar in 90 parts of deionized water, adding 0.5 parts of maleic acid dihydrazide and stirring at 45° C. for 2.5 hours, centrifuging or filtering, washing and purifying with water and ethanol, and then freeze-drying to obtain hydrazide-modified agar;

[0040] Step 2, dissolving 5 parts of graphene in 70 parts of deionized water by mass, adding 6 parts of L-cysteine, stirring and reacting at 50° C. for 1.5 hours, centrifuging or filtering, washing with water and ethanol for purification, and freeze-drying to obtain a conductive filler;

[0041] Step 3: Dissolve 6 parts of acrylamide in 70 parts of deionized water by mass, stir and dissolve at 60°C, then add 4 parts of isodecyl acrylate, 0.08 parts of crosslinker MBA, 4 parts of formaldehyde-modified agar, 3 parts of hydrazide-modified agar and 4 parts of conductive filler, react at 55°C with N2 for 2 hours, add 0.3 parts of initiator, and react at 65°C for 2 hours to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

[0042] Example 4

[0043] This embodiment provides a method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, comprising the following steps:

[0044] Step 1, dissolving 7 parts of guar gum in 80 parts of deionized water by mass, adding 4 parts of hydrogen peroxide and stirring at 40° C. for 4 hours, filtering, washing and drying to obtain aldehyde-modified guar gum; dissolving 7 parts of guar gum in 80 parts of deionized water, adding 0.3 parts of oxalic acid dihydrazide and stirring at 40° C. for 3 hours, centrifuging or filtering, washing and purifying with water and ethanol, and then freeze-drying to obtain hydrazide-modified guar gum;

[0045] Step 2, dissolving 6 parts of multi-walled carbon nanotubes in 80 parts of deionized water by mass, adding 4 parts of L-cysteine, stirring and reacting at 45° C. for 2 hours, centrifuging or filtering, washing with water and ethanol for purification, and freeze-drying to obtain a conductive filler;

[0046] Step 3: Dissolve 7 parts of acrylamide in 80 parts of deionized water by mass, stir and dissolve at 60°C, then add 2 parts of isobutyl acrylate, 0.06 parts of crosslinker MBA, 5 parts of formaldehyde-modified guar gum, 5 parts of hydrazide-modified guar gum and 5 parts of conductive filler, react at 60°C with N2 for 1 hour, add 0.4 parts of initiator sodium persulfate dropwise, and react at 70°C for 2 hours to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

[0047] Example 5

[0048] This embodiment provides a method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, comprising the following steps:

[0049] Step 1, dissolving 8 parts of pectin in 90 parts of deionized water by mass, adding 5 parts of ferric chloride oxide and stirring at 40° C. for 4 hours, filtering, washing and drying to obtain aldehyde-modified pectin; dissolving 8 parts of pectin in 90 parts of deionized water, adding 0.4 parts of p-nitrobenzoic hydrazide and stirring at 40° C. for 3 hours, centrifuging or filtering, washing and purifying with water and ethanol, and then freeze-drying to obtain hydrazide-modified pectin;

[0050] Step 2, dissolving 4 parts of silicon carbide fiber in 90 parts of deionized water by mass, adding 5 parts of polydopamine, stirring and reacting at 45° C. for 2 hours, centrifuging or filtering, washing with water and ethanol for purification, and freeze-drying to obtain a conductive filler;

[0051] Step 3: Dissolve 8 parts of acrylamide in 90 parts of deionized water by mass, stir and dissolve at 55°C, then add 3 parts of octyl methacrylate, 0.07 parts of crosslinker MBA, 4 parts of formaldehyde-modified pectin, 5 parts of hydrazide-modified pectin and 2 parts of conductive filler, react at 60°C with N2 for 1 hour, add 0.5 parts of initiator sodium persulfate dropwise, and react at 70°C for 2 hours to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

[0052] Example 6

[0053] This embodiment provides a method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, comprising the following steps:

[0054] Step 1, dissolving 2 parts of lignin in 70 parts of deionized water by mass, adding 4 parts of sodium hypochlorite and stirring at 40° C. for 4 hours, filtering, washing and drying to obtain aldehyde-modified lignin; dissolving 2 parts of lignin in 70 parts of deionized water, adding 0.3 parts of adipic acid dihydrazide and stirring at 40° C. for 3 hours, centrifuging or filtering, washing and purifying with water and ethanol, and then freeze-drying to obtain hydrazide-modified lignin;

[0055] Step 2, dissolving 2 parts of graphene oxide in 70 parts of deionized water by mass, adding 4 parts of reducing agent L-cysteine, stirring and reacting at 45° C. for 2 hours, centrifuging or filtering, washing with water and ethanol for purification, and freeze-drying to obtain a conductive filler;

[0056] Step 3: Dissolve 3 parts of acrylamide in 70 parts of deionized water by mass, stir and dissolve at 50°C, then add 3 parts of isobutyl methacrylate, 0.06 parts of crosslinker MBA, 3 parts of formaldehyde-treated lignin, 6 parts of hydrazide-treated lignin and 3 parts of conductive fillers, react at 60°C with N2 for 1 hour, add 0.3 parts of initiator potassium persulfate dropwise, and react at 70°C for 2 hours to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

[0057] The performance tests of the self-healing conductive hydrogel materials based on dynamic acylhydrazone bonds and hydrogen bonds prepared in the above Examples 1-6 were carried out as follows:

[0058] 1. Self-healing performance test:

[0059] The self-healing properties of the hydrogels prepared in Examples 1-6 were quantitatively characterized, and tensile tests were performed on the hydrogels before and after self-healing. First, a long strip of 35 mm × 4 mm × 4 mm hydrogel was prepared in a homemade mold. Then, the hydrogels before and after cutting were subjected to tensile tests to quantitatively characterize the self-healing behavior of the hydrogels. The tensile performance test results are shown in Table 1.

[0060] Table 1 Tensile strength test results

[0061]

[0062] Figure 1 and Figure 2 This is a real picture of the self-healing performance test of Example 1. It can be seen from the figure that the hydrogel prepared in Example 1 has good self-healing performance.

[0063] The self-healing efficiency of the hydrogels prepared in Examples 1-6 was calculated using the following formula:

[0064] Self-healing efficiency (%) = H t / H o ×100%

[0065] H o : Undamaged original tensile strength (KPa); H t :Tensile strength after repair (KPa).

[0066] The self-healing efficiency test results are shown in Table 2.

[0067] Table 2 Self-healing efficiency test results

[0068]

[0069] It can be seen from Tables 1 and 2 that the self-repairing performance of the self-repairing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds of the present invention can reach more than 85%, which shows that the self-repairing conductive hydrogel has good repair performance.

[0070] 2. Conductivity test:

[0071] The conductivity of the hydrogel prepared in Examples 1-6 was tested as follows: The conductivity of the material was tested by an electrochemical workstation. The conductive hydrogel was cut into 35 mm × 4 mm × 4 mm samples and fixed and clamped at both ends of the electrode clamp, and the voltage was set to 1.5 V. The conductivity (σ) of the hydrogel sample was calculated as follows:

[0072] σ=d / (R×A)

[0073] d: distance between adjacent electrodes (mm); R: resistance of hydrogel sample (Ω); A: cross-sectional area of ​​hydrogel sample (mm 2 ).

[0074] The test results of electrical conductivity are shown in Table 3.

[0075] Table 3 Conductivity test results

[0076]

[0077] It can be seen from Table 3 that the conductive properties of the self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds of the present invention are shown, which indicates that the self-healing conductive hydrogel has good conductive properties and can effectively and accurately transmit electrical signals when applied to strain sensors.

[0078] 3. Strain sensing performance test:

[0079] The strain sensing performance of the hydrogels prepared in Examples 1-6 was tested as follows: a digital multimeter was connected to a universal tensile testing machine, and a conductive hydrogel sample of 35 mm × 4 mm × 4 mm was first clamped at both ends of the tensile machine and connected to the wires of the digital multimeter to test the relative resistance change and sensitivity of the hydrogel sample under different strains. The strain was set to 150% and the voltage was set to 1.5 V. The sensitivity calculation formula of the hydrogel is as follows:

[0080] GF=(ΔR / R0) / ε

[0081] ε: applied strain; R0: initial resistance of the hydrogel sample; R: resistance under applied stress.

[0082] Table 4 Strain sensing performance test results

[0083] Performance Indicators Example 1 Example 2 Example 3 Example 4 Example 5 Example 6 Sensitivity 2.0 1.8 2.7 2.5 2.3 2.5

[0084] It can be seen from Table 4 that the sensitivity factor of the self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds of the present invention is greater than 1.5 when the strain is as small as 150%, which means that the conductive hydrogel has excellent strain sensitivity and a wide response range and can be applied to strain sensors.

[0085] In summary, the present invention is a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, wherein natural polysaccharides are modified by oxidants and hydrazide modifiers to obtain aldehyde-modified polysaccharides and hydrazide-modified polysaccharides, wherein the aldehyde group and the hydrazide group react to form an acylhydrazone bond, and then acrylamide, a hydrophobic monomer, and a carbon-based conductive filler are introduced, and a hydrogel material with stable conductive properties and excellent self-healing properties is successfully prepared by a free radical polymerization method. It is applied to strain sensors, which have the characteristics of high sensitivity and a wide response range, and can detect aspects such as human movement and health.

[0086] The above contents are only for explaining the technical idea of ​​the present invention and cannot be used to limit the protection scope of the present invention. Any changes made on the basis of the technical solution in accordance with the technical idea proposed by the present invention shall fall within the protection scope of the claims of the present invention.

Claims

1. A method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds, characterized in that: The following steps are involved: Step 1, dissolving 2 to 8 parts of natural polysaccharide in 70 to 90 parts of deionized water by mass, adding 4 to 6 parts of oxidant, stirring at 30 to 50° C. for 2 to 4 hours, separating the solid, washing, and drying to obtain the aldehyde-modified polysaccharide; dissolving 2 to 8 parts of natural polysaccharide in 70 to 90 parts of deionized water, adding 0.3 to 0.5 parts of hydrazide modifier, stirring at 35 to 45° C. for 2 to 3 hours, separating the solid, washing, and drying to obtain the hydrazide-modified polysaccharide; Step 2: Dissolve 2 to 6 parts of carbon-based material in 70 to 90 parts of deionized water by mass, add 4 to 6 parts of reducing agent, stir and react at 40 to 50° C. for 1 to 2 hours, separate the solid, wash and dry to obtain a conductive filler; Step three, dissolve 3 to 8 parts of acrylamide in 70 to 90 parts of deionized water by mass, stir and dissolve at 50 to 60°C, then add 2 to 4 parts of hydrophobic monomer, 0.06 to 0.08 parts of cross-linking agent MBA and 2 to 5 parts of aldehyde-modified polysaccharide prepared in step one, 1 to 6 parts of hydrazide-modified polysaccharide prepared in step one and 2 to 5 parts of conductive filler prepared in step two, react at 50 to 60°C with N2 for 1 to 3 hours, add 0.1 to 0.5 parts of initiator dropwise, and react at 60 to 70°C for 1 to 2 hours to obtain a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds.

2. The method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds according to claim 1, characterized in that: The natural polysaccharide includes any one of pectin, guar gum, starch, agar and lignin.

3. The method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds according to claim 1, characterized in that: The oxidant includes any one of sodium periodate, sodium hypochlorite, hydrogen peroxide and ferric oxychloride.

4. The method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds according to claim 1, characterized in that: The hydrazide modifier includes any one of adipic acid dihydrazide, succinic acid dihydrazide, maleic acid dihydrazide and p-nitrobenzoic acid hydrazide.

5. The method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds according to claim 1, characterized in that: The carbon-based material includes any one of graphene, graphene oxide, silicon carbide fiber, carbon powder and multi-walled carbon nanotubes.

6. The method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds according to claim 1, characterized in that: The reducing agent includes any one of polydopamine, sodium sulfite and L-cysteine.

7. The method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds according to claim 1, characterized in that: The hydrophobic monomer includes any one of octadecyl methacrylate, isooctyl acrylate, isobutyl acrylate, isodecyl acrylate, isobutyl methacrylate and octyl methacrylate.

8. The method for preparing a self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds according to claim 1, characterized in that: The initiator includes one of sodium persulfate, ammonium persulfate and potassium persulfate.

9. A self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds prepared by the method according to any one of claims 1 to 8.

10. Use of the self-healing conductive hydrogel material based on dynamic acylhydrazone bonds and hydrogen bonds as claimed in claim 9 in a flexible strain sensor.

Citation Information

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