A composite polyacrylamide gel electrolyte, its preparation method and application

Abstract

This invention discloses a composite polyacrylamide gel electrolyte, its preparation method, and its application. The preparation method of the composite polyacrylamide gel electrolyte includes the following steps: (1) using acrylamide as a raw material, N,N'-methylenebisacrylamide as a crosslinking agent, and deionized water as a solvent, adding an initiator and stirring until homogeneous to form solution A; (2) using Zn... 2+ Ba 2+ Or Al 3+ As a coordinating ion, it is dissolved in deionized water and stirred evenly to form solution B; (3) a natural polymer is added to solution B and stirred under inert gas protection to form solution C; (4) solution C is added to solution A and stirred under inert gas protection to form solution D; (5) solution D is polymerized to obtain a gel; (6) the gel is placed in an electrolyte for ion exchange to obtain a composite polyacrylamide gel electrolyte. This invention aims to enhance the mechanical strength of the gel electrolyte by introducing a tough ion-coordinating natural polymer material into the PAM polymer backbone.

Description

Technical fields:

[0001] This invention relates to the field of electrolyte technology, specifically to a composite polyacrylamide gel electrolyte, its preparation method, and its application. Background technology:

[0002] With the rapid development of global technology, flexible wearable electronic devices, due to their small size, lightweight convenience, and adaptable shape, have wide applications in information, medical, energy, and defense fields, becoming a major force driving human civilization and technological progress. Flexible energy storage devices, as the core component of wearable devices, have attracted widespread attention due to their high energy density and stable batteries. Electrolytes, as a key component of batteries, are essential carriers for ion transport during charging and discharging. Traditional electrolytes are mostly liquid electrolytes, which can lead to leakage, gas expansion, and other dangerous situations when electronic devices are subjected to different mechanical forces such as folding, bending, and compression, rendering the devices inoperable. Based on comprehensive considerations of safety and flexibility, using gel polymer electrolytes to replace liquid electrolytes is one of the important research directions for the development of flexible wearable electronic devices.

[0003] Compared to traditional organic electrolyte lithium-ion batteries, aqueous batteries have attracted attention from researchers both domestically and internationally in recent years due to their advantages such as low cost, high safety, and environmental friendliness. However, in aqueous battery systems, water, as the electrolyte, is prone to hydrogen evolution and oxygen evolution reactions on the electrode surface, causing battery expansion and significantly increasing safety hazards during device use.

[0004] To address the safety issues of aqueous batteries, gel polymer electrolytes, which have low water content and high ionic conductivity, have shown great potential. Compared to the traditional membrane-electrolyte structure, gel electrolytes are materials with a three-dimensional network structure. They can block electrons and conduct ions in the battery system, replacing the original "electrolyte + membrane" structure and simplifying the device composition. Therefore, they are more advantageous in constructing flexible devices. Compared to traditional electrolytes, gel electrolytes also have the following advantages: (1) They prevent electrolyte leakage and improve the safety performance of the device; (2) They have good flexibility and can withstand greater mechanical forces (bending, squeezing, impact) to meet different usage requirements; (3) They have a rich pore structure, which ensures ion transport; (4) They have viscosity, which improves the interfacial strength between the electrode and the electrolyte and effectively reduces the occurrence of delamination under strain.

[0005] Typically, gel polymer electrolytes are composed of a polymer matrix material, solvent, salt, and additives. Through polymer coagulation, the polymer network structure can maintain its original structure and performance stability even when moisture is absorbed. Furthermore, as a quasi-solid-state electrolyte, gel polymer electrolytes also possess high ionic conductivity similar to liquid electrolytes and self-supporting properties similar to solid electrolytes. Therefore, gel electrolytes have received widespread attention in recent years, especially in the field of aqueous zinc-ion batteries. Currently, the most representative gel electrolytes used in aqueous zinc-ion batteries include polyvinyl alcohol (PVA)-based, polyacrylic acid (PAA)-based, and polyacrylamide (PAM)-based electrolytes. PVA, due to its abundant hydroxyl groups, possesses excellent water absorption properties. PVA also has advantages such as self-healing, good chemical stability, low cost, and non-toxicity, and has been widely used in flexible devices. For example, zinc-ion batteries using PVA / zinc trifluoromethanesulfonate as the electrolyte have shown extremely strong repair capabilities after being cut, completely restoring battery performance. PAA, with its unique structural characteristics, can absorb a large number of water molecules, improving ionic conductivity; however, its poor mechanical strength has become a bottleneck in its commercialization. PAM, due to its simple preparation conditions, high water content, and high conductivity, has become an ideal electrolyte material for flexible devices. However, compared to PAA and PVA, the presence of amide groups in the PAM structure makes its tensile properties difficult to meet application requirements. To improve the mechanical properties of PAM, SiO2 nanoparticles can be used as fillers to effectively improve the tensile strength of PAM; however, the poor interfacial compatibility between PAM and inorganic materials restricts its development. Summary of the Invention:

[0006] This invention addresses the problems existing in the prior art, providing a composite polyacrylamide gel electrolyte, its preparation method, and its applications. This invention enhances the mechanical strength of the gel electrolyte by introducing a tough, ion-coordinated natural polymer material into the PAM polymer backbone. Simultaneously, the abundant functional groups in the natural polymer material effectively alleviate the problem of poor interfacial compatibility between the filler and the substrate.

[0007] The purpose of this invention is to provide a method for preparing a composite polyacrylamide gel electrolyte, comprising the following steps:

[0008] (1) Using acrylamide as raw material, N,N'-methylenebisacrylamide as crosslinking agent, deionized water as solvent, and sodium persulfate, ammonium persulfate or potassium persulfate as initiator, mix and stir the above substances until a homogeneous solution A is formed.

[0009] (2) With Zn 2+ Ba 2+ Or Al 3+As a coordinating ion, zinc salt, barium salt or aluminum salt is dissolved in deionized water and stirred until a homogeneous solution B is formed.

[0010] (3) Add natural polymer to solution B obtained in step (2), and stir rapidly under inert gas protection until a homogeneous solution C is formed;

[0011] (4) Slowly add solution C to solution A obtained in step (1), and stir under inert gas protection to form a homogeneous solution D;

[0012] (5) The solution D obtained in step (4) is polymerized to obtain a gel;

[0013] (6) The gel after polymerization in step (5) is placed in an electrolyte for ion exchange to obtain a composite polyacrylamide gel electrolyte.

[0014] In step (1), acrylamide is dissolved in deionized water to form an acrylamide solution of 0.1 to 0.5 g / mL. In step (3), rapid stirring refers to stirring at a speed of 380 to 420 rpm. In step (4), slow addition of solution C refers to adding solution C at a speed of 0.9 to 1.1 mL / min.

[0015] Preferably, the crosslinking agent in step (1) accounts for 0.1% to 0.5% of the mass of acrylamide, and the initiator accounts for 0.1% to 0.5% of the mass of acrylamide.

[0016] Preferably, the concentration of the coordinating ions in solution B in step (2) is 5.0–10.0 g / L. The zinc salt, barium salt, or aluminum salt is preferably zinc nitrate (Zn(NO3)2), barium nitrate (Ba(NO3)2), or aluminum nitrate (Al(NO3)3).

[0017] Preferably, the natural polymer in solution C in step (3) is selected from sodium alginate, cellulose and starch, and the mass ratio of coordinating ions to natural polymers is 2 to 3:1.

[0018] Preferably, the inert gas in step (3) or (4) is nitrogen or argon. An inert gas must be introduced into the uniform dispersion C or dispersion D in step (3) or (4) to form a homogeneous and transparent solution under the protection of the inert gas.

[0019] Preferably, the natural polymer in step (4) accounts for 2% to 5% of the mass of acrylamide.

[0020] Preferably, the polymerization reaction conditions in step (5) are as follows: first, the temperature is increased to 40℃~50℃ at a heating rate of 5℃ / min, and the polymerization reaction is carried out for 1~2 hours; then, the temperature is increased to 75℃~80℃ at a heating rate of 5℃ / min, and the polymerization reaction is carried out for 5~6 hours.

[0021] Preferably, the electrolyte in step (6) contains zinc sulfate with a concentration of 2.0 mol / L and manganese sulfate with a concentration of 0.1 mol / L, and the ion exchange time is 4.0 to 12.0 h.

[0022] This invention also protects the composite polyacrylamide gel electrolyte obtained by the above preparation method. The ion-coordination type natural polymer / PAM composite gel electrolyte provided by this invention can enhance the orderliness between natural polymer materials and improve the mechanical tensile strength of the gel electrolyte through the coordination of ions with natural polymers.

[0023] This invention also protects the application of the above-mentioned composite polyacrylamide gel electrolyte as an electrolyte in a battery, including aqueous batteries such as zinc-ion batteries and aluminum-ion batteries.

[0024] Preferably, the battery is an aqueous zinc-ion battery.

[0025] Compared with the prior art, the present invention has the following advantages:

[0026] (1) The present invention uses ion-coordinated natural polymers as reinforcing agents. Through the coordination of ions and natural polymers, the covalent interaction between PAM and natural polymers, and the hydrogen bonding between natural polymers and PAM, the synergistic effect of the three endows PAM gel electrolyte with excellent mechanical properties.

[0027] (2) The tensile strength of the ion coordination type natural polymer / PAM composite gel electrolyte prepared by the present invention can reach 180-300 MPa.

[0028] (3) The natural polymer materials used in this invention are abundant, renewable and degradable, which helps to reduce the production cost of the device and is also conducive to achieving environmental friendliness and sustainable development.

[0029] (4) The ion coordination type natural polymer / PAM composite gel electrolyte proposed in this invention adopts a programmed temperature polymerization method during the polymerization process. This method can meet the different requirements of different materials in the composite for polymerization temperature, which is different from the previous polymerization at a single temperature. Attached image description:

[0030] Figure 1 Al obtained in Example 1 3+ Infrared spectrum of coordination-type SA / PAM composite gel electrolyte;

[0031] Figure 2 These are Al samples of different qualities from Examples 1-4. 3+ Comparison of the effects of coordination type SA on the tensile strength of PAM composite gel electrolyte;

[0032] Figure 3 The graph shows the performance of the zinc-ion battery with the SA / PAM composite gel electrolyte obtained in Comparative Example 1.

[0033] Figure 4 Al obtained in Example 1 3+ Performance graph of zinc-ion battery with coordination-type SA / PAM composite gel electrolyte;

[0034] Figure 5 The Al obtained in Example 1, Comparative Example 1, and Comparative Example 2 3+ Coordination-type SA / PAM complex gel, SA / PAM complex gel, Al 3+ Comparison of tensile strength of modified PAM composite gel electrolyte;

[0035] Figure 6 These are Al samples of different qualities from Examples 5-8. 3+ Comparison of the effects of coordination type CN on the tensile strength of PAM composite gel electrolyte;

[0036] Figure 7 This is a comparison chart of the tensile strength of SA / PAM composite gel electrolytes with different coordination ions obtained in Examples 1, 9, and 10. Detailed implementation method:

[0037] The following embodiments are further illustrations of the present invention, but not limitations thereof.

[0038] Unless otherwise defined, all technical terms used herein have the same meaning as commonly understood by those skilled in the art. The technical terms used herein are for the purpose of describing particular embodiments only and are not intended to limit the scope of the invention. Unless otherwise specified, the experimental materials and reagents used herein are commercially available products conventionally available in this technical field.

[0039] Example 1

[0040] An SA / PAM composite gel electrolyte is prepared by the following steps:

[0041] (1) Using acrylamide as raw material, N,N'-methylenebisacrylamide as crosslinking agent, deionized water as solvent, and sodium persulfate as initiator, a certain amount of acrylamide is dissolved in deionized water to form an acrylamide solution of 0.1 g / mL. Then, N,N'-methylenebisacrylamide and sodium persulfate are added and ultrasonically stirred until a homogeneous solution A is formed, wherein N,N'-methylenebisacrylamide accounts for 0.1% of the mass of acrylamide and sodium persulfate accounts for 0.1% of the mass of acrylamide.

[0042] (2) Using aluminum nitrate (Al(NO3)3) as the coordinating ion and deionized water as the solvent, aluminum nitrate was dissolved in deionized water and ultrasonicated and stirred until a homogeneous solution B was formed. The aluminum nitrate in solution B... 3+ The concentration of the coordinating ion is 5.0 g / L.

[0043] (3) Add sodium alginate (SA) to the uniformly dispersed solution B, and stir rapidly under nitrogen protection until a homogeneous solution C is formed. The coordinating ion Al in solution C is... 3+ It accounts for 300% of the mass of sodium alginate.

[0044] (4) Slowly add solution C to the uniformly dispersed solution A, and stir for a certain time under nitrogen protection to form a uniform solution D, in which sodium alginate accounts for 2% of the mass of acrylamide.

[0045] (5) Transfer solution D to the mold and place it in a programmed temperature drying oven. Polymerize at a certain temperature for a certain time to obtain gel. The conditions for the polymerization reaction are: first, polymerize at a heating rate of 5℃ / min at a temperature of 40℃ for 2 hours, and then polymerize at a heating rate of 5℃ / min at a temperature of 80℃ for 6 hours.

[0046] (6) Place the polymerized gel from step (5) in an electrolyte for ion exchange. After a certain period of time, Al can be obtained. 3+ A coordination-type SA / PAM composite gel electrolyte, wherein the electrolyte contains zinc sulfate at a concentration of 2.0 mol / L and manganese sulfate at a concentration of 0.1 mol / L, and the ion exchange time is 12 h.

[0047] The Al prepared above 3+ The coordination-type SA / PAM composite gel electrolyte was characterized and its performance was analyzed. Figure 1 It is Al 3+ The infrared spectrum of the coordination-type sodium alginate (SA) / polyacrylamide (PAM) composite gel electrolyte shows that at 3468 cm⁻¹... -1 1654cm -1 1458cm -1 1110cm -1 618cm -1 Peaks were observed for NH stretching vibration, C=O stretching vibration, CH2 scissor vibration, CO stretching, and NH out-of-plane rocking vibration; these characteristic peaks are all attributed to PAM characteristics. At 2920 cm⁻¹ -1 1600cm -1 1410cm -1 1030cm -1The peaks for the asymmetric stretching vibrations of CH, the asymmetric and symmetric stretching vibrations of COO, and the stretching vibration of CO were observed, all of which belong to SA. The infrared spectrum confirms that Al... 3+ Formation of a coordination-type SA / PAM complex gel electrolyte. ICP testing revealed Al... 3+ The proportion is 297%, which is close to the feed ratio of 300%.

[0048] Examples 2-4

[0049] Same as Example 1, except that in step (4), sodium alginate accounts for 3%, 4%, and 5% of the mass of acrylamide, respectively.

[0050] Figure 2 These are Al samples of different qualities from Examples 1-4. 3+ Comparison of the effects of coordination type SA on the tensile strength of PAM composite gel electrolyte, respectively, with Al 3+ Coordinating SA was added to polyacrylamide at different masses (2%, 3%, 4%, 5%). A comparison showed that Al... 3+ The addition of coordination-type SA can improve the tensile strength of PAM gel. When the addition amount is 2%, the tensile strength of the composite gel electrolyte is 180 MPa, and when the addition amount is increased to 5%, the tensile strength of the composite gel electrolyte is 300 MPa.

[0051] Comparative Example 1

[0052] An SA / PAM composite gel electrolyte is prepared by the following steps:

[0053] (1) Using acrylamide as raw material, N,N'-methylenebisacrylamide as crosslinking agent, deionized water as solvent, and sodium persulfate as initiator, acrylamide is dissolved in deionized water to form an acrylamide solution of 0.1 g / mL. Then, N,N'-methylenebisacrylamide and sodium persulfate are added and ultrasonically stirred until a homogeneous solution A is formed, wherein N,N'-methylenebisacrylamide accounts for 0.1% of the mass of acrylamide and sodium persulfate accounts for 0.1% of the mass of acrylamide.

[0054] (2) Add sodium alginate to a uniformly dispersed solution A, and stir for a certain time under nitrogen protection to form a uniform solution D, wherein sodium alginate accounts for 8% of the mass of acrylamide.

[0055] (3) Transfer solution D to a mold and place it in a programmed temperature drying oven. Polymerize at a certain temperature for a certain time to obtain a gel. The conditions for the polymerization reaction are: first, polymerize at a heating rate of 5℃ / min at a temperature of 40℃ for 2 hours, and then polymerize at a heating rate of 5℃ / min at a temperature of 80℃ for 6 hours.

[0056] (4) The polymerized gel in step (3) is placed in an electrolyte for ion exchange. After a certain period of time, an SA / PAM composite gel electrolyte can be prepared. The electrolyte contains 2.0 mol / L zinc sulfate and 0.1 mol / L manganese sulfate, and the ion exchange time is 12 h.

[0057] Figure 3 The zinc-ion battery assembled using the SA / PAM composite gel obtained in Comparative Example 1 as the electrolyte, zinc sheet as the negative electrode, and manganese dioxide as the positive electrode can be seen from the figure. The results show that when the current density is 1.0 Ag... -1 2.0Ag -1 5.0Ag -1 At that time, its specific capacity was 282.4 mAh g. -1 253.8mAh g -1 218.6mAh g -1 When Al obtained in Example 1 3+ The performance of zinc-ion batteries assembled with coordination-type SA / PAM gel electrolytes, from... Figure 4 As can be seen from the image, when the current density is 1.0Ag -1 2.0Ag -1 5.0Ag -1 At that time, its specific capacity was 306.2 mAh g. -1 268.8mAh g -1 227.5mAh g -1 This result shows that, compared to SA / PAM composite gel electrolytes, Al 3+ Coordination-type SA / PAM electrolytes are more conducive to improving the performance of zinc-ion batteries.

[0058] Comparative Example 2

[0059] A gel electrolyte is prepared by the following steps:

[0060] (1) Using acrylamide as raw material, N,N'-methylenebisacrylamide as crosslinking agent, deionized water as solvent, and sodium persulfate as initiator, a certain amount of acrylamide is dissolved in deionized water to form an acrylamide solution of 0.1 g / mL. Then, N,N'-methylenebisacrylamide and sodium persulfate are added and ultrasonically stirred until a homogeneous solution A is formed, wherein N,N'-methylenebisacrylamide accounts for 0.1% of the mass of acrylamide and sodium persulfate accounts for 0.1% of the mass of acrylamide.

[0061] (2) Using aluminum nitrate (Al(NO3)3) as the coordinating ion and deionized water as the solvent, aluminum nitrate was dissolved in deionized water and ultrasonicated and stirred until a homogeneous solution B was formed. The aluminum nitrate in solution B...3+ The concentration of the coordinating ion is 5.0 g / L.

[0062] (3) Slowly add solution B to the uniformly dispersed solution A, and stir for a certain period of time under nitrogen protection to form a uniform solution D, in which Al 3+ It accounts for 8% of the mass of acrylamide.

[0063] (4) Transfer solution D to the mold and place it in a programmed temperature drying oven. Polymerize at a certain temperature for a certain time to obtain gel. The conditions for the polymerization reaction are: first, polymerize at a heating rate of 5℃ / min at a temperature of 40℃ for 2 hours, and then polymerize at a heating rate of 5℃ / min at a temperature of 80℃ for 6 hours.

[0064] (5) Place the polymerized gel from step (4) in an electrolyte for ion exchange. After a certain period of time, Al can be obtained. 3+ A coordination-type SA / PAM composite gel electrolyte, wherein the electrolyte contains 2.0 mol / L zinc sulfate and 0.1 mol / L manganese sulfate, and the ion exchange time is 12 h.

[0065] Figure 5 This is a comparison chart of the tensile strength of three gel electrolytes: Example 1, Comparative Example 1, and Comparative Example 2. The comparison shows that, with Al... 3+ When SA is used as a filler, the tensile strength of the composite gel electrolyte is 180 MPa, which is significantly higher than that of SA and Al alone. 3+ Tensile strength of PAM gels with coordinating ions.

[0066] Example 5

[0067] A CN / PAM composite gel electrolyte is prepared by the following steps:

[0068] (1) Using acrylamide as raw material, N,N'-methylenebisacrylamide as crosslinking agent, deionized water as solvent, and sodium persulfate as initiator, acrylamide is dissolved in deionized water to form an acrylamide solution of 0.1 g / mL. Then, N,N'-methylenebisacrylamide and sodium persulfate are added and ultrasonically stirred until a homogeneous solution A is formed, wherein N,N'-methylenebisacrylamide accounts for 0.1% of the mass of acrylamide and sodium persulfate accounts for 0.1% of the mass of acrylamide.

[0069] (2) Using aluminum nitrate (Al(NO3)3) as the coordinating ion and deionized water as the solvent, aluminum nitrate was dissolved in deionized water and ultrasonicated and stirred until a homogeneous solution B was formed, in which Al 3+ The concentration of the coordinating ion is 5.0 g / L.

[0070] (3) Add cellulose (CN) to the uniformly dispersed solution B, and stir rapidly under nitrogen protection until a homogeneous solution C is formed, with the coordination ion Al 3+ It accounts for 100% of the mass of natural polymers.

[0071] (4) Slowly add solution C to the uniformly dispersed solution A, and stir for a certain time under nitrogen protection to form a uniform solution D, in which the natural polymer accounts for 2% of the mass of acrylamide.

[0072] (5) Transfer solution D to a mold and place it in a programmed temperature drying oven. Polymerize at a certain temperature for a certain time to obtain a gel. The polymerization conditions are as follows: first, polymerize at a heating rate of 5℃ / min at a temperature of 40℃ for 2 hours, and then polymerize at a heating rate of 5℃ / min at a temperature of 80℃ for 6 hours.

[0073] (6) Place the polymerized gel from step (5) in an electrolyte for ion exchange. After a certain period of time, Al can be prepared. 3+ A coordination-type CN / PAM composite gel electrolyte, wherein the electrolyte contains 2.0 mol / L zinc sulfate and 0.1 mol / L manganese sulfate, and the ion exchange time is 12 h.

[0074] Examples 6-8

[0075] Same as Example 5, except that in step (4), cellulose accounts for 3%, 4%, and 5% of the mass of acrylamide, respectively.

[0076] Figure 6 These are Al samples of different qualities from Examples 5-8. 3+ A comparative diagram showing the effect of coordination cellulose (CN) on the tensile strength of PAM composite gel electrolytes, with Al... 3+ Coordinating CN was added to PAM at different masses (2%, 3%, 4%, 5%). The comparison showed that the addition of coordinating CN could improve the tensile strength of PAM. When the addition amount was 5%, the tensile strength of the composite gel electrolyte was 298 MPa.

[0077] Example 9

[0078] Similar to Example 1, except that in step (2), barium nitrate (Ba(NO3)3) is used as the coordinating ion.

[0079] Example 10

[0080] Similar to Example 1, except that zinc nitrate (Zn(NO3)3) is used as the coordinating ion in step (2).

[0081] Figure 7These are different coordination ions (Al) obtained in Examples 1, 9, and 10. 3+ Ba 2+ Zn 2+ A comparative figure showing the effect of modified SA on the tensile strength of PAM composite gel electrolytes, with Al being modified accordingly. 3+ Ba 2+ Zn 2+ When coordinated SA is added to polyacrylamide, a comparison shows that Al 3+ The addition of coordination-type SA significantly improves the tensile strength of PAM gel, which reaches 180 MPa, significantly higher than that of Ba. 2+ PAM gel with coordination type SA (172 MPa) and Zn 2+ PAM gel with coordinating ions (177 MPa).

[0082] The above description of the embodiments is only for the purpose of helping to understand the technical solution and core idea of ​​the present invention. It should be noted that for those skilled in the art, several improvements and modifications can be made to the present invention without departing from the principle of the present invention, and these improvements and modifications also fall within the protection scope of the claims of the present invention.

Claims

1. A method for preparing a composite polyacrylamide gel electrolyte, characterized in that, Includes the following steps: (1) Using acrylamide as raw material, N,N'-methylenebisacrylamide as crosslinking agent, deionized water as solvent, and sodium persulfate, ammonium persulfate or potassium persulfate as initiator, mix and stir the above substances until a homogeneous solution A is formed; (2) With Al 3+ As a coordinating ion, the aluminum salt is dissolved in deionized water and stirred until a homogeneous solution B is formed. (3) Add natural polymer to solution B obtained in step (2), stir under inert gas protection until a homogeneous solution C is formed. The natural polymer is selected from sodium alginate, cellulose and starch, and the mass ratio of coordinating ion to natural polymer is 2~3:

1. (4) Add solution C to solution A obtained in step (1), and stir under inert gas protection to form a homogeneous solution D; (5) The solution D obtained in step (4) is polymerized to obtain a gel. The polymerization reaction conditions are as follows: firstly, at 5... o The temperature was increased to 40℃~50℃ at a heating rate of C / min, and the polymerization reaction was carried out for 1~2 h, then at 5℃... o The temperature was increased to 75℃~80℃ at a heating rate of C / min, and the polymerization reaction was carried out for 5~6 h. (6) The gel after polymerization in step (5) is placed in an electrolyte for ion exchange to obtain a composite polyacrylamide gel electrolyte.

2. The preparation method according to claim 1, characterized in that, The crosslinking agent mentioned in step (1) accounts for 0.1% to 0.5% of the mass of acrylamide, and the initiator accounts for 0.1% to 0.5% of the mass of acrylamide.

3. The preparation method according to claim 1 or 2, characterized in that, The concentration of the coordinating ions in solution B described in step (2) is 5.0~10.0 g / L.

4. The preparation method according to claim 1 or 2, characterized in that, The inert gas mentioned in step (3) or (4) is nitrogen or argon.

5. The preparation method according to claim 1 or 2, characterized in that, The natural polymers mentioned in step (4) account for 2% to 5% of the mass of acrylamide.

6. The preparation method according to claim 1, characterized in that, The electrolyte in step (6) contains zinc sulfate with a concentration of 2.0 mol / L and manganese sulfate with a concentration of 0.1 mol / L, and the ion exchange time is 4.0~12 h.

7. The composite polyacrylamide gel electrolyte obtained by the preparation method according to claim 1.

8. The application of the composite polyacrylamide gel electrolyte of claim 7 as a battery electrolyte, characterized in that, The battery in question is an aqueous zinc-ion battery.

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