Preparation methods and applications of graphene oxide-based interpenetrating network polymer hydrogels and their electrodes

Abstract

This invention provides a method for preparing a graphene oxide-based interpenetrating polymer network (IPN) hydrogel, which mainly includes the following steps: First, graphene oxide is prepared using a modified Hummers method; then, using acrylic acid as a monomer and graphene oxide as a framework, a polyacrylic acid / graphene oxide IPN hydrogel is obtained by polymerization; utilizing the amino groups on the graphene oxide as active sites, pyrrole is grafted onto the IPN hydrogel to obtain a polyacrylic acid / graphene oxide-grafted polypyrrole IPN hydrogel; the graphene oxide-based IPN hydrogel can be used as an electrode material for flexible supercapacitors.

Description

Technical Field

[0001] This invention relates to a method for preparing a graphene oxide-based interpenetrating polymer hydrogel electrode, belonging to the fields of functional polymer materials and electrochemistry. Background Art

[0002] In recent years, flexible electronic devices have developed rapidly, such as foldable displays and pulse sensors. To meet the needs of flexible electronic devices, the focus is on developing thin, lightweight electronic devices with excellent electrochemical performance. Due to their advantages such as high power density, long lifespan, high safety, and ease of integration with other systems, supercapacitors have attracted increasing attention in wearable power supply applications. A key technology for wearable supercapacitors is the preparation of electrode materials, currently used materials include carbon-based materials, metal oxides, and conductive polymers. Although carbon-based materials (such as carbon nanotubes and graphene) have good conductivity and flexibility, their inherent double-layer charge storage behavior results in low specific capacitance. Metal oxides, as electrode materials, can provide high energy storage capacitance, but their brittleness and poor conductivity limit their application in wearable supercapacitors. Conductive polymers, due to their good mechanical toughness and thin film fabrication characteristics, are promising electrode materials for flexible supercapacitors. Improving the specific capacitance of electrode materials has become a hot research topic for scientists.

[0003] Graphene is a type of poly(phosphorus) material. 2 Graphene is a novel material composed of hybridized carbon atoms tightly packed into a single-layer two-dimensional honeycomb lattice structure. Due to its superior electrical conductivity, photon transmission performance, and excellent mechanical properties, it shows broad application prospects in supercapacitors, adsorbent materials, biomedical materials, lithium-ion batteries, and aerospace materials. Research on graphene has entered a phase of rapid development, and graphene has become a "star" material among today's new materials. A key research area is how to combine graphene with conductive polymers to improve the specific capacitance of the material. For example, Chen Guo et al. uniformly dispersed graphene in an aqueous solution containing aniline, added an initiator to prepare polyaniline, and uniformly encapsulated graphene in polyaniline to form a blend material. At a current density of 0.5 A / g, the specific capacitance of graphene oxide / polyaniline was 419 F / g, which was significantly improved compared with pure polyaniline (381 F / g). Even at a high current density of 5 A / g, it still maintained a high specific capacitance (360 F / g) (Cheng Guo et al. Preparation and properties of dye-modified graphene oxide / polyaniline composites, Polymer Materials Science and Engineering, 2010, 31, 175). Summary of the Invention

[0004] The purpose of this invention is to provide a method for preparing and using graphene oxide-based interpenetrating polymer hydrogels and their electrodes, in order to solve the above-mentioned problems existing in the prior art.

[0005] To achieve the above objectives, the technical solution of the present invention is as follows:

[0006] A method for preparing a graphene oxide-based interpenetrating polymer hydrogel includes the following steps:

[0007] S1. Graphene oxide is dispersed in distilled water, and acrylic acid, N,N-methylenebisacrylamide and ammonium persulfate are added. After mixing, a polymerization reaction is initiated by ultraviolet light under nitrogen protection to obtain polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel.

[0008] S2. Modify the polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel with concentrated ammonia to obtain polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel.

[0009] S3. The polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel is mixed with pyrrole, isopropanol, distilled water and hydrochloric acid. Then, under ice-water bath conditions, an aqueous solution of ammonium persulfate is added to carry out the reaction to obtain polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel, that is, the graphene oxide-based interpenetrating network polymer hydrogel.

[0010] As a preferred embodiment, the method for preparing the graphene oxide is as follows:

[0011] After mixing flake graphite and phosphoric acid, concentrated sulfuric acid and potassium permanganate were added under ice-water bath conditions. After reacting for 2 hours, the temperature was raised to 40-60℃ and the reaction was continued for 1 hour. After cooling to room temperature, ice water was added and stirred. Then, 30% hydrogen peroxide was added dropwise. The mixture was filtered, washed, and vacuum dried to obtain graphene oxide.

[0012] As a preferred embodiment, the mass ratio of the flake graphite, phosphoric acid and potassium permanganate is (1-2):(4-5):(3-5).

[0013] As a preferred embodiment, the wavelength of the ultraviolet light mentioned in step S1 is 365nm.

[0014] As a preferred embodiment, the mass ratio of graphene oxide to acrylic acid is (1-2):(4-10).

[0015] As a preferred option, the specific operation of step S2 is as follows:

[0016] Polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel was mixed with 24% concentrated ammonia water and subjected to a hydrothermal reaction at 90-100℃. After cooling, filtration, washing with distilled water and vacuum drying, polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel was obtained.

[0017] As a preferred embodiment, the mass ratio of the polyacrylic acid / amino modified graphene oxide interpenetrating network polymer hydrogel to pyrrole is (1-2):(3-6).

[0018] A method for preparing a graphene oxide-based interpenetrating polymer hydrogel electrode includes the following steps:

[0019] The aforementioned polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel, acetylene black, and PTFE were ultrasonically dispersed in ethanol, coated onto nickel foam, and vacuum dried at 60°C for 6 hours. Then, the hydrogel electrode was prepared by pressing it under a pressure of 10 MPa, which is the graphene oxide-based interpenetrating network hydrogel electrode.

[0020] The use of a graphene oxide-based interpenetrating network polymer hydrogel electrode obtained by the aforementioned preparation method in flexible supercapacitor electrode materials.

[0021] The basic principle of this invention is as follows:

[0022] 1. First, graphene oxide is prepared using the improved Hummers method, mainly by using phosphoric acid instead of nitric acid. This results in mild reaction conditions and the absence of any toxic gases. At the same time, a large number of epoxy groups are introduced onto the graphene oxide, which facilitates the subsequent reaction with ammonia to generate amino-modified graphene oxide.

[0023] 2. Using acrylic acid as the monomer, N,N-methylenebisacrylamide as the crosslinking agent, ammonium persulfate as the initiator, and graphene oxide as the backbone, a polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel was obtained by polymerization.

[0024] 3. Under heating and pressurization conditions, ammonia water is used to open the epoxy groups on graphene oxide, allowing the amino groups to directly connect with the graphene oxide, thus obtaining a polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel.

[0025] 4. Using the amino groups on graphene oxide as active sites, pyrrole is grafted and copolymerized onto the interpenetrating network polymer hydrogel to obtain polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel.

[0026] Compared with the prior art, the present invention has the following beneficial effects:

[0027] 1. By utilizing the high porosity and large specific surface area of ​​graphene oxide, pyrrole is grafted onto its surface, which greatly increases the specific surface area of ​​the hydrogel and improves the specific capacitance of the material.

[0028] 2. Grafting pyrrole onto graphene oxide yields graphene oxide-grafted polypyrrole. Polypyrrole and graphene form a P-π conjugated structure, allowing electrons to be transferred between graphene and the conductive polymer polypyrrole. This facilitates the formation of continuous conductive channels in the hydrogel network, significantly improving the material's conductivity.

[0029] 3. Using graphene oxide as a backbone, acrylic acid monomer is immersed in the backbone and polymerized to obtain polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel. Compared with ordinary composites, interpenetrating network polymer has superior electrical and mechanical properties.

[0030] 4. The specific capacitance of the polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel is composed of double-layer capacitance and Faraday pseudocapacitance, which greatly improves the specific capacitance of the electrode.

[0031] 5. The conductive hydrogel prepared by this invention has the characteristics of stable preparation process, easy operation, low equipment dependence, and no pollution, making it suitable for large-scale industrial production and promising to become an ideal electrode material for flexible supercapacitors. Attached Figure Description

[0032] Other features, objects, and advantages of the present invention will become more apparent from the following detailed description of non-limiting embodiments with reference to the accompanying drawings:

[0033] Figure 1 This is a scanning electron microscope image of the graphene oxide-based interpenetrating network polymer hydrogel prepared in this invention. Detailed Implementation

[0034] The present invention will now be described in detail with reference to specific embodiments. These embodiments will help those skilled in the art to further understand the present invention, but do not limit the invention in any way. It should be noted that those skilled in the art can make various modifications and improvements without departing from the concept of the present invention. These all fall within the scope of protection of the present invention.

[0035] Example 1

[0036] This embodiment provides a method for preparing a graphene oxide-based interpenetrating network hydrogel electrode, which specifically includes the following steps:

[0037] 1. Preparation of graphene oxide

[0038] 1.0 g of flake graphite and 4 g of phosphoric acid were added to a three-necked flask. The flask was placed in an ice-water bath, and 20 mL of concentrated sulfuric acid was slowly added. The mixture was magnetically stirred for 10 min, and then 3.5 g of potassium permanganate was slowly added. The reaction was allowed to proceed for 2 h. The temperature was raised to 50 °C and the reaction was continued for 1 h. After cooling to room temperature, 100 mL of ice water was added to the reaction solution, and the mixture was stirred. 1 mL of hydrogen peroxide (30% by mass) was added dropwise. The mixture was then filtered, washed, and dried under vacuum to obtain graphene oxide.

[0039] 2. Preparation of polyacrylic acid / graphene oxide interpenetrating network polymer hydrogels

[0040] 0.7 g of graphene oxide was dispersed in 10 g of distilled water to obtain a graphene oxide dispersion. 3.0 g of acrylic acid (AA), 0.04 g of N,N-methylenebisacrylamide (MBA), and 0.05 g of ammonium persulfate were added to the dispersion, and the mixture was magnetically stirred at room temperature. Under nitrogen protection, the mixture was irradiated under a 365 nm UV lamp for 10 min to obtain a polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel.

[0041] 3. Preparation of polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogels

[0042] 0.5 g of polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel was added to a 20 mL pressure reactor, and then the reactor was filled with 24% concentrated ammonia water. The reaction was carried out at 95 °C for 6 h. After cooling, the mixture was filtered, washed with distilled water, and dried under vacuum to obtain polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel.

[0043] 0.5 g of polyacrylic acid / amino-modified graphene oxide, 4 mL of isopropanol, 20 mL of distilled water, 60 mL of 2 mol / mL hydrochloric acid solution, and 1.5 g of pyrrole were added to a three-necked flask. The flask was placed in an ice-water bath, and then 30 g of 10% ammonium persulfate aqueous solution was slowly added. The mixture was stirred and reacted for 6 h. After filtration, washing, and vacuum drying, a polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel was obtained.

[0044] 4. Preparation of polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrodes

[0045] Polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel, acetylene black, and PTFE were mixed in anhydrous ethanol at a mass ratio of 8:1:1. After ultrasonic dispersion for 40 min, the mixture was coated onto nickel foam and vacuum dried at 60 °C for 6 h. Then, the mixture was pressed into a sheet under a pressure of 10 MPa to obtain the polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrode, namely the graphene oxide-based interpenetrating network hydrogel electrode.

[0046] The morphology of the graphene oxide-based interpenetrating network hydrogel electrode prepared in Example 1 is as follows: Figure 1 As shown, the hydrogel has a porous structure with pore sizes of approximately 5-10 μm. The hydrogel has a porosity of 95.1% and a specific surface area of ​​17.2 m². 2 The conductivity is 2.1 S / m. Under a current density of 1 A / g, the specific capacitance is 210 F / g.

[0047] Example 2

[0048] This embodiment provides a method for preparing a graphene oxide-based interpenetrating network hydrogel electrode, which specifically includes the following steps:

[0049] 1. Preparation of graphene oxide

[0050] 1.2 g of flake graphite and 4.5 g of phosphoric acid were added to a three-necked flask, which was then placed in an ice-water bath. 20 mL of concentrated sulfuric acid was slowly added, and the mixture was magnetically stirred for 10 min. 4 g of potassium permanganate was then slowly added, and the reaction was allowed to proceed for 2 h. The temperature was raised to 50 °C, and the reaction was continued for 1 h. After cooling to room temperature, 100 mL of ice water was added to the reaction mixture, and the mixture was stirred. 1 mL of hydrogen peroxide (30% by mass) was added dropwise. The mixture was then filtered, washed, and vacuum dried to obtain graphene oxide.

[0051] 2. Preparation of polyacrylic acid / graphene oxide interpenetrating network polymer hydrogels

[0052] 0.6 g of graphene oxide was dispersed in 10 g of distilled water to obtain a graphene oxide dispersion. 3.2 g of acrylic acid (AA), 0.04 g of N,N-methylenebisacrylamide (MBA), and 0.05 g of ammonium persulfate were added to the dispersion, and the mixture was magnetically stirred at room temperature. Under nitrogen protection, the mixture was irradiated under a 365 nm UV lamp for 10 min to obtain a polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel.

[0053] 3. Preparation of polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogels

[0054] 0.5 g of polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel was added to a 20 mL pressure reactor, and then the reactor was filled with 24% concentrated ammonia water. The reaction was carried out at 95 °C for 6 h. After cooling, the mixture was filtered, washed with distilled water, and dried under vacuum to obtain polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel.

[0055] 0.7 g of polyacrylic acid / amino-modified graphene oxide, 4 mL of isopropanol, 20 mL of distilled water, 60 mL of 2 mol / mL hydrochloric acid solution, and 2 g of pyrrole were added to a three-necked flask. The flask was placed in an ice-water bath, and then 30 g of 10% ammonium persulfate aqueous solution was slowly added. The mixture was stirred and reacted for 6 h. After filtration, washing, and vacuum drying, a polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel was obtained.

[0056] 4. Preparation of polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrodes

[0057] Polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel, acetylene black, and PTFE were mixed in anhydrous ethanol at a mass ratio of 8:1:1. After ultrasonic dispersion for 40 min, the mixture was coated onto nickel foam and vacuum dried at 60 °C for 6 h. Then, the mixture was pressed into a sheet under a pressure of 10 MPa to obtain the polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrode, namely the graphene oxide-based interpenetrating network hydrogel electrode.

[0058] The graphene oxide-based interpenetrating network hydrogel electrode prepared in Example 2 has a porosity of 93.9% and a specific surface area of ​​15.2 m². 2 The conductivity is 2.2 S / m. Under a current density of 1 A / g, the specific capacitance is 219 F / g.

[0059] Example 3

[0060] This embodiment provides a method for preparing a graphene oxide-based interpenetrating network hydrogel electrode, which specifically includes the following steps:

[0061] 1. Preparation of graphene oxide

[0062] 0.9 g of flake graphite and 4.5 g of phosphoric acid were added to a three-necked flask, which was then placed in an ice-water bath. 20 mL of concentrated sulfuric acid was slowly added, and the mixture was magnetically stirred for 10 min. 3.6 g of potassium permanganate was then slowly added, and the reaction was allowed to proceed for 2 h. The temperature was raised to 50 °C, and the reaction was continued for 1 h. After cooling to room temperature, 100 mL of ice water was added to the reaction solution, and the mixture was stirred. 1 mL of hydrogen peroxide (30% by mass) was added dropwise. The mixture was then filtered, washed, and vacuum dried to obtain graphene oxide.

[0063] 2. Preparation of polyacrylic acid / graphene oxide interpenetrating network polymer hydrogels

[0064] 0.5 g of graphene oxide was dispersed in 10 g of distilled water to obtain a graphene oxide dispersion. 2.8 g of acrylic acid (AA), 0.04 g of N,N-methylenebisacrylamide (MBA), and 0.05 g of ammonium persulfate were added to the dispersion, and the mixture was magnetically stirred at room temperature. Under nitrogen protection, the mixture was irradiated under a 365 nm UV lamp for 10 min to obtain a polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel.

[0065] 3. Preparation of polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogels

[0066] 0.5 g of polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel was added to a 20 mL pressure reactor, and then the reactor was filled with 24% concentrated ammonia water. The reaction was carried out at 95 °C for 6 h. After cooling, the mixture was filtered, washed with distilled water, and dried under vacuum to obtain polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel.

[0067] 0.75 g of polyacrylic acid / amino-modified graphene oxide, 4 mL of isopropanol, 20 mL of distilled water, 60 mL of 2 mol / mL hydrochloric acid solution, and 2.2 g of pyrrole were added to a three-necked flask. The flask was placed in an ice-water bath, and then 30 g of 10% ammonium persulfate aqueous solution was slowly added. The mixture was stirred and reacted for 6 h. After filtration, washing, and vacuum drying, a polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel was obtained.

[0068] 4. Preparation of polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrodes

[0069] Polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel, acetylene black, and PTFE were mixed in anhydrous ethanol at a mass ratio of 8:1:1. After ultrasonic dispersion for 40 min, the mixture was coated onto nickel foam and vacuum dried at 60 °C for 6 h. Then, the mixture was pressed into a sheet under a pressure of 10 MPa to obtain the polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrode, namely the graphene oxide-based interpenetrating network hydrogel electrode.

[0070] The graphene oxide-based interpenetrating network hydrogel electrode prepared in Example 3 has a porosity of 94.1% and a specific surface area of ​​16.9 m². 2 The conductivity is 1.9 S / m. Under a current density of 1 A / g, the specific capacitance is 211 F / g.

[0071] Comparative Example 1

[0072] Unlike Example 1, step 1) is omitted. In step 2), "flake graphite" is directly used instead of "graphene oxide" to finally obtain a polyacrylic acid / flake graphite grafted polypyrrole interpenetrating network polymer hydrogel. This hydrogel has a porosity of 63.1% and a specific surface area of ​​1.2 m². 2 The conductivity is 0.8 S / m. Under a current density of 1 A / g, the specific capacitance is 79 F / g.

[0073] Comparative Example 2

[0074] Unlike Example 1, step 2) is omitted, and in step 3) "graphene oxide" is used instead of "polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel," ultimately yielding graphene oxide-grafted polypyrrole. This material has a porosity of 88.1% and a specific surface area of ​​16.0 m². 2 The conductivity is 1.8 S / m. Under a current density of 1 A / g, the specific capacitance is 181 F / g.

[0075] Comparative Example 3

[0076] Unlike Example 1, the amino modification step 3) is omitted. The polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel prepared in step 2) is not amino modified and is directly used for polymerization with pyrrole. Since the graphene oxide is not amino modified, pyrrole cannot be grafted onto it and can only polymerize via self-homogeneity, ultimately yielding a polyacrylic acid / graphene oxide / polypyrrole interpenetrating network polymer hydrogel. This hydrogel has a porosity of 90.1% and a specific surface area of ​​15.1 m². 2 The conductivity is 0.9 S / m. Under a current density of 1 A / g, the specific capacitance is 119 F / g.

[0077] The specific embodiments of the present invention have been described above. It should be understood that the present invention is not limited to the specific embodiments described above, and those skilled in the art can make various modifications or variations within the scope of the claims, which do not affect the essence of the present invention.

Claims

1. A method for preparing a polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel electrode, characterized in that, Includes the following steps: Polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel, acetylene black, and PTFE were ultrasonically dispersed in ethanol, coated onto nickel foam, vacuum dried at 60°C for 6 h, and then pressed into sheets under 10 MPa pressure to obtain polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrodes. The preparation method of the polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel includes the following steps: S1. Disperse graphene oxide in distilled water, add acrylic acid, N,N Methylenebisacrylamide and ammonium persulfate were mixed and then polymerized under nitrogen protection using ultraviolet light to obtain a polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel. S2. Modify the polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel with concentrated ammonia to obtain polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel. S3. The polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel is mixed with pyrrole, isopropanol, distilled water and hydrochloric acid. Then, under the condition of ice water bath, ammonium persulfate aqueous solution is added to carry out the reaction to obtain polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel, that is, the polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel. The wavelength of the ultraviolet light mentioned in step S1 is 365 nm.

2. The method for preparing the polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel electrode as described in claim 1, characterized in that, The preparation method of the graphene oxide is as follows: After mixing flake graphite and phosphoric acid, concentrated sulfuric acid and potassium permanganate were added under ice-water bath conditions. After reacting for 2 hours, the temperature was raised to 40-60℃ and the reaction was continued for 1 hour. After cooling to room temperature, ice water was added and stirred. Then, 30% hydrogen peroxide was added dropwise. The mixture was filtered, washed, and vacuum dried to obtain graphene oxide.

3. The method for preparing the polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrode as described in claim 2, characterized in that, The mass ratio of the flake graphite, phosphoric acid and potassium permanganate is (1~2):(4~5):(3~5).

4. The method for preparing the polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrode as described in claim 1, characterized in that, The mass ratio of graphene oxide to acrylic acid is (1~2):(4~10).

5. The method for preparing the polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel electrode as described in claim 1, characterized in that, The specific operation of step S2 is as follows: Polyacrylic acid / graphene oxide interpenetrating network polymer hydrogel was mixed with 24% concentrated ammonia water and subjected to a hydrothermal reaction at 90~100℃. After cooling, filtration, washing with distilled water and vacuum drying, polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel was obtained.

6. The method for preparing the polyacrylic acid / graphene oxide grafted polypyrrole interpenetrating network polymer hydrogel electrode as described in claim 1, characterized in that, The mass ratio of the polyacrylic acid / amino-modified graphene oxide interpenetrating network polymer hydrogel to pyrrole is (1~2):(3~6).

7. The use of a polyacrylic acid / graphene oxide-grafted polypyrrole interpenetrating network polymer hydrogel electrode obtained by the preparation method of claim 1 in flexible supercapacitor electrode materials.

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