A biomimetic ligament structure interpenetrating network hydrogel electrolyte and preparation and application thereof
By using an interpenetrating network hydrogel electrolyte with a biomimetic ligament structure, the problem of balancing mechanical strength and ion conductivity in flexible zinc-ion batteries has been solved, achieving stable electrochemical output of high-performance zinc-ion batteries under complex deformation.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- GUIZHOU UNIV
- Filing Date
- 2026-02-04
- Publication Date
- 2026-05-29
AI Technical Summary
Existing flexible zinc-ion batteries with aqueous electrolytes suffer from problems such as difficulty in balancing mechanical strength and ion conductivity, poor long-term deformation recovery, and insufficient ability to suppress zinc dendrite growth and interfacial side reactions.
The interpenetrating network hydrogel electrolyte with a biomimetic ligament structure mimics the microstructure and composition characteristics of human ligaments to construct a composite system in which flexible polymer networks and rigid nanofiber networks interpenetrate each other. By combining chemical crosslinking and physical crosslinking, a network structure rich in multifunctional functional groups is formed.
It achieves high tensile strength, high toughness and excellent fatigue recovery performance, maintains extremely high ionic conductivity and zinc ion transference number, suppresses zinc dendrite growth and side reactions, and ensures stable electrochemical output of the battery under complex deformation.
Smart Images
Figure CN122118124A_ABST
Abstract
Description
Technical Field
[0001] This invention belongs to the field of electrochemical energy storage materials and flexible electronics technology, specifically relating to a high-performance interpenetrating network hydrogel electrolyte with a biomimetic ligament structure, its preparation method, and its application in flexible zinc-ion batteries. More specifically, this invention relates to a hydrogel electrolyte system that achieves synergistic improvement in mechanical and electrochemical performance by simulating the microstructure and functional group distribution of human ligaments. Background Technology
[0002] Flexible aqueous zinc-ion batteries (FZIBs) are favored for their high safety, environmental friendliness, low cost, and the high theoretical capacity of zinc metal (820 mAh g⁻¹). -1 Zinc-ion batteries (FZIBs) have shown broad application prospects in wearable electronic devices, flexible displays, and electronic skin. However, traditional aqueous electrolytes are prone to uncontrolled dendrite growth during zinc-ion battery cycling, leading to internal short circuits. Simultaneously, the hydrogen evolution reaction, corrosion reaction, and byproduct formation associated with aqueous electrolytes further deteriorate the electrode-electrolyte interface stability, severely impacting battery cycle life. Furthermore, the insufficient flexibility of traditional aqueous electrolytes significantly hinders their development in flexible aqueous zinc-ion batteries. Therefore, developing a flexible electrolyte to suppress these side reactions and dendrite growth is crucial for achieving high-performance and stable FZIBs.
[0003] Currently, most flexible electrolytes address flexibility issues by developing hydrogel electrolytes. However, traditional hydrogel electrolytes generally face a trade-off between mechanical and electrochemical properties. Some current improvement strategies include: 1. Introducing high-valence metal ions to enhance the cross-linking network, but this may lead to gel brittleness, and the metal ions may interfere with electrochemical reactions. 2. Adding biomolecular frameworks to improve biocompatibility and certain functionalities, but the mechanical enhancement effect is limited when used alone, and the regulation of ion transport is not precise enough. 3. Introducing small-molecule additives to regulate electrochemical behavior, but their contribution to overall mechanical properties is minimal. These methods often only improve one aspect of performance and struggle to achieve excellent mechanical toughness, rapid recovery ability, and effective control of the zinc deposition process while maintaining high ionic conductivity.
[0004] In nature, biological tissues have evolved over millions of years, achieving highly optimized structure and function. Human ligaments, a typical load-bearing soft tissue, consist of a flexible proteoglycan matrix interwoven with rigid collagen fibers, forming a unique interpenetrating network structure. This structure endows ligaments with extremely high toughness, excellent energy dissipation capacity, and structural stability under long-term repetitive stress. Inspired by this, introducing this "flexible-rigid" interpenetrating network concept into hydrogel electrolyte design holds promise for breaking through traditional performance limitations. Furthermore, natural biomolecules are rich in various polar functional groups. If these groups can be systematically integrated into the network, not only can abundant dynamic physical cross-linking points be constructed to enhance mechanical properties, but these functional groups can also be used to precisely control the solvation structure and interfacial electrochemical environment of the electrolyte.
[0005] Therefore, developing an integrated hydrogel electrolyte with a biomimetic ligament structure, excellent mechanical properties, efficient and stable ion transport, and zinc deposition regulation capability is key to promoting the practical application of flexible zinc-ion batteries.
[0006] Currently, there are no reports of hydrogel electrolytes designed based on this biomimetic concept and successfully applied to high-performance flexible zinc-ion batteries. Summary of the Invention
[0007] In view of the problems existing in flexible zinc-ion batteries with hydrogel electrolytes, such as the difficulty in balancing mechanical strength and ion conductivity, poor long-term deformation recovery, and insufficient ability to suppress zinc dendrite growth and interfacial side reactions, this invention provides a novel biomimetic ligament-structured interpenetrating network hydrogel electrolyte and its preparation method. This electrolyte aims to achieve the following objectives by mimicking the microstructure and compositional characteristics of human ligaments: 1. Achieve high tensile strength, high toughness, and excellent fatigue recovery performance close to that of biological ligaments.
[0008] 2. Maintain extremely high ionic conductivity and zinc ion transport number to ensure the ion transport rate in the battery.
[0009] 3. By utilizing the abundant functional groups in the network structure, the zinc ion solvation structure can be regulated, and the distribution of ions and electron fields on the electrode surface can be homogenized, thereby fundamentally inhibiting the growth of zinc dendrites and the occurrence of side reactions.
[0010] 4. Ensure that the assembled flexible battery can maintain stable electrochemical output under complex deformations such as bending and folding.
[0011] The technical solution of the present invention: To achieve the above objectives, the present invention adopts the following technical solution: I. Composition and Structural Design of Hydrogel Electrolytes This invention provides a biomimetic ligament-structured interpenetrating network hydrogel electrolyte, the core of which lies in constructing a composite system rich in multifunctional functional groups, consisting of an interpenetrating flexible polymer network and a rigid nanofiber network. Specifically, it comprises the following components: Component 1: Polymerizable acrylic protonated chitosan ionic liquid; Component 2: Zinc salt; Component 3: Acrylic acid and its derivative monomers; Component 4: Functionalized cellulose nanofibers; The components form an interpenetrating network structure through the combined action of chemical and physical cross-linking.
[0012] The following three components are key: 1. Polymerizable acrylic protonated chitosan ionic liquid: as a flexible matrix phase and for functional regulation. Chitosan, after being protonated with acrylic acid, forms a polymerizable ionic liquid. The cationic groups it provides can effectively regulate the deposition behavior of zinc ions.
[0013] 2. Acrylic acid and its derivative monomers: serving as the main body of the flexible framework. The polymer network formed by their polymerization provides the main elasticity and stretchability, and through chemical crosslinking and copolymerization with protonated chitosan, a first-layer flexible polymer network is formed.
[0014] 3. Functionalized cellulose nanofibers: Serving as a rigid reinforcement and functional regulator. After functionalization, cellulose is rich in functional groups on its surface. Through its nanofiber-like structure, it undergoes strong physical entanglement and hydrogen bonding with a flexible network, forming a second rigid network. It mimics the collagen fibers in ligaments, responsible for bearing and dispersing stress, significantly improving the strength, modulus, and toughness of the hydrogel. Furthermore, the carboxyl groups it provides can participate in regulating the solvation structure and deposition behavior of zinc ions.
[0015] Preferably, in the aforementioned biomimetic ligament structure interpenetrating network hydrogel electrolyte, the content of the functionalized cellulose nanofibers is 0.1-6% of the mass of water.
[0016] Preferably, in the aforementioned biomimetic ligament structure interpenetrating network hydrogel electrolyte, the zinc salt is one or more of zinc sulfate, zinc trifluoromethanesulfonate, zinc nitrate, zinc chloride, or zinc acetate in any proportion; the acrylic acid derivative monomer is one of acrylamide, methacrylate, N-hydroxyethylacrylamide, N,N-dimethylacrylamide, 2-acrylamido-2-methylpropanesulfonic acid, hydroxyethyl methacrylate, or methacrylic acid; and the functionalized cellulose nanofibers are one of TEMPO oxidized cellulose nanofibers, sulfonated cellulose nanofibers, phosphorylated cellulose nanofibers, or quaternized cellulose nanofibers.
[0017] Preferably, in the aforementioned biomimetic ligament structure interpenetrating network hydrogel electrolyte, the concentration of acrylic acid and its derivative monomers is 150-500 g / L, the concentration of zinc salt is 1-8 mol / L, and the concentration of polymerizable acrylic protonated chitosan ionic liquid is 10-60 g / L.
[0018] II. Preparation methods of hydrogel electrolytes A method for preparing a biomimetic ligament structure interpenetrating network hydrogel electrolyte includes the following steps: Step 1: Dissolve chitosan in an aqueous solution of acrylic acid to obtain a polymerizable protonated chitosan ionic liquid; Step 2: Add zinc salt, acrylic acid and its derivative monomers and functionalized cellulose nanofibers to the liquid obtained in Step 1 and disperse them evenly by ultrasonication; Step 3: Add crosslinking agent and initiator to the liquid obtained in step 2, stir evenly, and carry out polymerization reaction at a constant temperature for a period of time to form a biomimetic ligament structure interpenetrating network hydrogel electrolyte.
[0019] Preferably, in the aforementioned method for preparing the biomimetic ligament structure interpenetrating network hydrogel electrolyte, the crosslinking agent is N'N'-methylenebisacrylamide; and the initiator is ammonium persulfate.
[0020] Preferably, in the aforementioned method for preparing the biomimetic ligament structure interpenetrating network hydrogel electrolyte, the concentration of the crosslinking agent added is 0.01-2 g / L, and the concentration of the initiator added is 0.2-3 g / L.
[0021] Preferably, in the aforementioned method for preparing the biomimetic ligament structure interpenetrating network hydrogel electrolyte, in step 3, the constant temperature is 40-90℃ and the polymerization time is 0.5-4h.
[0022] III. A zinc-ion battery Based on the same inventive concept, the present invention also provides the application of the hydrogel electrolyte prepared by the above method in flexible zinc-ion batteries and electrolytes for wearable electronic devices. The hydrogel electrolyte can be used to prepare high-performance zinc symmetric batteries, zinc-copper batteries, zinc-manganese dioxide full batteries or flexible pouch batteries.
[0023] 1. This invention integrates polymerizable acrylic protonated chitosan ionic liquid, acrylic acid derivative monomers, and functionalized cellulose nanofibers to prepare a biomimetic ligament-structured interpenetrating network hydrogel electrolyte for high-performance and stable zinc ionized water (FZIBs). This strategy mimics the structure of biological ligaments to form a rigid-flexible interpenetrating network. The flexible network ensures large deformation capacity and continuity of ion transport channels, while the rigid network provides mechanical support and energy dissipation sites, greatly improving mechanical stability. Furthermore, the functional groups distributed throughout the network can precisely promote zinc ion transport, regulate the zinc ion solvation structure, and homogenize the electric field and ion concentration on the electrode surface, thereby achieving uniform zinc deposition. Therefore, the hydrogel exhibits excellent mechanical properties and stable electrochemical performance.
[0024] 2. This invention innovatively introduces the concept of ligament biomimicry into electrolyte design, solving the industry problem that it is difficult to synergistically improve the mechanical and electrochemical properties of hydrogel electrolytes.
[0025] 3. This invention achieves performance optimization of electrolyte materials at three levels: macroscopic mechanics, microscopic ion transport, and interfacial electrochemistry through a dual strategy of "rigid-flexible interpenetrating network" and "synergistic use of multifunctional groups".
[0026] 4. The preparation method of this invention is simple, the raw materials are widely available, it is environmentally friendly, easy to scale up production, and has good commercialization prospects.
[0027] 5. The biomimetic ligament structure interpenetrating network hydrogel electrolyte provided by this invention has a zinc ion transference number as high as 0.727 and an ionic conductivity as high as 23.98 mS / cm. -1 .
[0028] 6. The biomimetic ligament structure interpenetrating network hydrogel electrolyte provided by this invention has a stable cycle life of over 2400 hours at room temperature, high coulombic efficiency and excellent specific capacity when applied to zinc-ion batteries.
[0029] 7. The biomimetic ligament structure interpenetrating network hydrogel electrolyte provided by the present invention, together with the FZIBs composed of the electrolyte, MnO2@CC cathode and zinc anode, can provide stable and continuous power supply for electronic timers under harsh environments with different bending states. Attached Figure Description
[0030] Figure 1 The PCILM-2CNF-gel hydrogel electrolyte obtained in Example 2 of this invention has an elongation at break of 3068% and a tensile strength of 183 kPa.
[0031] Figure 2The PCILM-2CNF-gel hydrogel electrolyte obtained in Example 2 of this invention was subjected to a loading and unloading cycle test under 500% strain. After standing for 20 minutes, its maximum stress recovered to 96.4% of the initial value, and the hysteresis loop area recovered to 98.1%.
[0032] Figure 3 The ion transference number of the PCILM-2CNF-gel hydrogel electrolyte obtained in Example 2 of this invention is 0.727.
[0033] Figure 4 For the zinc symmetric batteries assembled with electrolytes obtained in Comparative Examples 1, 2, 2, and 6 of this invention, the current density is 1 mA cm⁻¹. -2 and a capacity density of 1 mAh cm⁻¹ -2 SEM images after 100 cycles clearly show that AE, PAM-gel, and PCILM-gel electrolytes have a large number of zinc dendrites growing on their surfaces, forming sharp cones; while the zinc anode surface of PCILM-2CNF-gel hydrogel electrolyte is relatively flat, and zinc dendrites preferentially grow along the (002) crystal plane.
[0034] Figure 5 Zinc symmetric batteries assembled with electrolytes obtained in Comparative Examples 1, 2, 2, and 6 of this invention were used at a current density of 1 mA cm⁻¹. -2 The capacity density is 1 mAh cm⁻¹ -2 The following is a graph showing the long-cycle performance. When using the PCILM-2CNF-gel hydrogel electrolyte, the zinc symmetric battery exhibits superior stability during cycling, achieving stable cycling for over 2400 hours and showing a significant improvement in lifespan, effectively enhancing the battery's long-cycle stability.
[0035] Figure 6 For Comparative Examples 1, 2, 2, and 6 of this invention, zinc-copper asymmetric batteries assembled with electrolytes were used at a current density of 2 mA cm⁻¹. -2 The capacity density is 0.5 mAh cm⁻¹. -2 The following is a graph showing the long-cycle performance. When using the PCILM-2CNF-gel hydrogel electrolyte, the zinc-copper asymmetric battery exhibits superior stability during cycling, achieving stable cycling for over 1300 cycles with an average coulombic efficiency of up to 99.3%.
[0036] Figure 7 The FZIBs, composed of the PCILM-2CNF-gel hydrogel electrolyte obtained in Example 2 of this invention, MnO2@CC cathode, and zinc anode, can provide stable and continuous power to the electronic timer under harsh environments with different bending states. Detailed Implementation
[0037] The present invention will be further described below with reference to embodiments, but these embodiments are not intended to limit the scope of the invention.
[0038] Comparative Example 1 11.21 g of ZnSO4 7H2O and 10 mL of deionized water were diluted to volume in a volumetric flask and dissolved completely at room temperature to obtain 2 M ZnSO4 aqueous electrolyte, denoted as AE.
[0039] Comparative Example 2 6g of acrylamide monomer, 11.21g of ZnSO4 7H2O and 20mL of deionized water were stirred thoroughly at room temperature. The mixture was then transferred to an oven at 40-90℃ for 0.5-3 hours to obtain PAM-gel hydrogel electrolyte. Example 1
[0040] Weigh 200 mg of chitosan powder (degree of deacetylation > 90%) and slowly add it to a beaker containing 20 mL of 0.5 wt% acrylic acid aqueous solution. Stir magnetically at room temperature for 4-8 hours until the chitosan is completely dissolved, resulting in a clear, slightly viscous, pale yellow solution, which is the polymerizable acrylic protonated chitosan ionic liquid, labeled as PCIL solution. Example 2
[0041] First, 11.21 g of ZnSO4·7H2O was weighed and added to the PCIL solution, and then stirred vigorously at room temperature for 12 hours. Subsequently, 6 g of acrylamide was added and stirred until completely dissolved. Then, 0.2% (666 μL) of TEMPO oxidized cellulose nanofibers were added, and the mixture was sonicated to obtain a homogeneous solution. Next, 3 mg of N,N-methylenebisacrylamide and 30 mg of ammonium persulfate were added to the sonicated solution. The mixture was transferred to a mold and polymerized in an oven at 40-90 °C for 0.5-3 hours to obtain the PCILM-2CNF-gel hydrogel electrolyte. Example 3
[0042] The steps are the same as in Example 2, except that the amount of TEMPO oxidized cellulose nanofibers is changed to 0.1% (333 μL), and other conditions remain unchanged, and PCILM-1CNF-gel hydrogel electrolyte is finally obtained. Example 4
[0043] The steps are the same as in Example 2, except that the amount of TEMPO oxidized cellulose nanofibers is changed to 0.3% (1000 μL), and other conditions remain unchanged, and PCILM-3CNF-gel hydrogel electrolyte is finally obtained. Example 5
[0044] The steps are the same as in Example 2, except that the amount of TEMPO oxidized cellulose nanofibers is changed to 0.4% (1333 μL), and other conditions remain unchanged, and PCILM-4CNF-gel hydrogel electrolyte is finally obtained. Example 6
[0045] The steps are the same as in Example 2, except that TEMPO oxidized cellulose nanofibers are not added, and other conditions remain unchanged, and PCILM-gel hydrogel electrolyte is finally obtained. Example 7
[0046] The steps are the same as in Example 2, except that the amount of TEMPO oxidized cellulose nanofibers is changed to 6%, and other conditions remain unchanged, and PCILM-60CNF-gel hydrogel electrolyte is finally obtained. Example 8
[0047] The steps are the same as in Example 2, except that the amount of acrylamide added is adjusted to 150 g / L, and other conditions remain unchanged, and the hydrogel electrolyte is finally obtained. Example 9
[0048] The steps are the same as in Example 2, except that the amount of acrylamide added is adjusted to 500 g / L, and other conditions remain unchanged, and the hydrogel electrolyte is finally obtained. Example 10
[0049] The steps are the same as in Example 2, except that the zinc salt is replaced with zinc nitrate and the amount added is adjusted to 1 mol / L, while other conditions remain unchanged, and finally a hydrogel electrolyte is obtained. Example 11
[0050] The steps are the same as in Example 2, except that the zinc salt is replaced with zinc acetate and the amount added is adjusted to 8 mol / L, while other conditions remain unchanged, and finally a hydrogel electrolyte is obtained. Example 12
[0051] The steps are the same as in Example 2, except that the concentration of PCIL in the homogeneous solution is 10 g / L. Example 13
[0052] The steps are the same as in Example 2, except that the concentration of PCIL in the homogeneous solution is 60 g / L. Example 14
[0053] The steps are the same as in Example 2, except that acrylamide is replaced with acrylic acid. Example 15
[0054] The steps are the same as in Example 2, except that acrylamide is replaced with methacrylate. Example 16
[0055] The steps are the same as in Example 2, except that acrylamide is replaced with N-hydroxyethylacrylamide. Example 17
[0056] The steps are the same as in Example 2, except that acrylamide is replaced with N,N-dimethylacrylamide. Example 18
[0057] The steps are the same as in Example 2, except that acrylamide is replaced with 2-acrylamide-2-methylpropanesulfonic acid. Example 19
[0058] The steps are the same as in Example 2, except that acrylamide is replaced with hydroxyethyl methacrylate. Example 20
[0059] The steps are the same as in Example 2, except that acrylamide is replaced with methacrylic acid. Example 21
[0060] The steps are the same as in Example 2, except that the TEMPO oxidized cellulose nanofibers are modified to sulfonated cellulose nanofibers. Example 22
[0061] The steps are the same as in Example 2, except that the TEMPO oxidized cellulose nanofibers are replaced with phosphorylated cellulose nanofibers. Example 23
[0062] The steps are the same as in Example 2, except that the TEMPO oxidized cellulose nanofibers are modified to quaternized cellulose nanofibers. Example 24
[0063] The hydrogel obtained in Example 2 was cut into standard dumbbell-shaped specimens and subjected to tensile testing using a universal testing machine. The results showed that its elongation at break was 3068% and its tensile strength was 183 kPa. After a loading and unloading cycle test at 500% strain and a resting period of 20 minutes, its maximum stress recovered to 96.4% of the initial value, and the hysteresis loop area recovered to 98.1%. Example 25
[0064] The hydrogel obtained in Example 2 was cut into circular slices and sandwiched between two stainless steel blocking electrodes. Its ionic conductivity was measured by electrochemical impedance spectroscopy and calculated to be 23.98 mS / cm at 25°C. -1 Zn was tested using the Bruce-Vincent method combined with DC polarization. 2+ The number of migrations is calculated. . Example 26
[0065] The hydrogel obtained in Example 2 was cut into circular slices, and coin cells were assembled using zinc foil as the two electrodes. At 1 mA cm⁻¹ -1 Current density, 1 mAh cm -2 The battery underwent constant current charge-discharge cycling at its capacity density and operated stably for over 2400 hours, maintaining stable overpotential. The battery was assembled using copper foil as the working electrode and zinc foil as the counter and reference electrodes. At 2 mA cm⁻¹ -2 0.5 mAhcm -2 Under the specified conditions, the coulombic efficiency was tested, with an average value of 99.3%, and it could be stably cycled 1300 times. A soft-pack battery was constructed using electrodeposited MnoO2 carbon cloth as the positive electrode and zinc foil as the negative electrode, encapsulated in an aluminum-plastic film. This battery could stably discharge under various conditions, including flat, 90° bent, and 180° bent states, continuously powering a small electronic timer, with no significant difference in the discharge curve.
[0066] The above description is merely a preferred embodiment of the present invention, but the scope of protection of the present invention is not limited thereto. Any equivalent substitutions or modifications made by those skilled in the art within the scope of the technology disclosed in the present invention, based on the technical solution and inventive concept of the present invention, should be covered within the scope of protection of the present invention.
Claims
1. A biomimetic ligament structure interpenetrating network hydrogel electrolyte, characterized in that, It contains the following components: Component 1: Polymerizable acrylic protonated chitosan ionic liquid; Component 2: Zinc salt; Component 3: Acrylic acid and its derivative monomers; Component 4: Functionalized cellulose nanofibers; The components form an interpenetrating network structure through the combined action of chemical and physical cross-linking.
2. The biomimetic ligament structure interpenetrating network hydrogel electrolyte according to claim 1, characterized in that: The content of the functionalized cellulose nanofibers is 0.1-6% of the mass of water.
3. The biomimetic ligament structure interpenetrating network hydrogel electrolyte according to claim 1, characterized in that: The zinc salt is one or more of zinc sulfate, zinc trifluoromethanesulfonate, zinc nitrate, zinc chloride, or zinc acetate in any proportion; the acrylic acid derivative monomer is one of acrylamide, methacrylate, N-hydroxyethylacrylamide, N,N-dimethylacrylamide, 2-acrylamido-2-methylpropanesulfonic acid, hydroxyethyl methacrylate, or methacrylic acid; the functionalized cellulose nanofiber is one of TEMPO oxidized cellulose nanofiber, sulfonated cellulose nanofiber, phosphorylated cellulose nanofiber, or quaternized cellulose nanofiber.
4. The biomimetic ligament structure interpenetrating network hydrogel electrolyte according to claim 1, characterized in that: The concentration of the acrylic acid and its derivative monomers is 150-500 g / L, the concentration of the zinc salt is 1-8 mol / L, and the concentration of the polymerizable acrylic protonated chitosan ionic liquid is 10-60 g / L.
5. A method for preparing a biomimetic ligament structure interpenetrating network hydrogel electrolyte according to any one of claims 1-4, characterized in that, Includes the following steps: Step 1: Dissolve chitosan in an aqueous solution containing acrylic acid to obtain a polymerizable protonated chitosan ionic liquid; Step 2: Add zinc salt, acrylic acid and its derivative monomers and functionalized cellulose nanofibers to the liquid obtained in Step 1 and disperse them evenly by ultrasonication; Step 3: Add crosslinking agent and initiator to the liquid obtained in step 2, stir evenly, and carry out polymerization reaction at a constant temperature to form a biomimetic ligament structure interpenetrating network hydrogel electrolyte.
6. The method for preparing the biomimetic ligament structure interpenetrating network hydrogel electrolyte according to claim 5, characterized in that: The crosslinking agent is N'N'-methylenebisacrylamide; the initiator is ammonium persulfate.
7. The method for preparing the biomimetic ligament structure interpenetrating network hydrogel electrolyte according to claim 5, characterized in that: The concentration of the crosslinking agent added is 0.01-2 g / L, and the concentration of the initiator added is 0.2-3 g / L.
8. The method for preparing the biomimetic ligament structure interpenetrating network hydrogel electrolyte according to claim 5, characterized in that: In step 3, the constant temperature is 40-90℃ and the polymerization time is 0.5-4h.
9. The application of a biomimetic ligament structure interpenetrating network hydrogel electrolyte according to any one of claims 1-4 in a zinc-ion battery.
10. A zinc-ion battery, characterized in that: The battery comprises the biomimetic ligament structure interpenetrating network hydrogel electrolyte as described in any one of claims 1-4; wherein the zinc-ion battery is a zinc symmetric battery, a zinc-copper battery, a zinc-manganese dioxide full battery, or a flexible pouch battery.