Two-dimensional stretchable supercapacitor based on viscous electrolyte and preparation method thereof

Abstract

The invention discloses a two-dimensional stretchable supercapacitor based on viscous electrolyte and a preparation method thereof, and belongs to the technical field of hydrogel materials. Semi-gel electrodes are embedded into semi-gel viscous electrolyte in a printing mode, and composite viscous gel composed of two parallel gel electrodes and the viscous gel electrolyte is named as the viscous multiphase gel supercapacitor. According to the invention, the nested viscous multiphase gel based on the viscous electrolyte is developed by using a bulk phase and interface synergetic energy dissipation strategy and is used for constructing the two-dimensional stretchable supercapacitor with ultrahigh strain, ultrahigh energy density and ultrahigh power density at the same time. According to the invention, the semi-gel electrode is embedded into the semi-gel viscous electrolyte in a printing manner to form the nested viscous multiphase gel supercapacitor, and the comprehensive performances such as stretchability and energy density of the two-dimensional supercapacitor (SCs) are improved by using a bulk phase and interface synergistic energy dissipation strategy.

Description

Technical Field

[0001] The present invention relates to the technical field of hydrogel materials, and in particular to a two-dimensional stretchable supercapacitor based on a viscous electrolyte and a preparation method thereof. Background Art

[0002] Compared with sandwich supercapacitors, two-dimensional supercapacitors (2D SCs) have the advantages of no need for external metal interconnection, integration, patterning, and miniaturization [LiF., Hu A., Zhao X., et al. On-chip high-energy interdigital micro-supercapacitors with 3D nanotubular array electrodes. J. Mater. Chem. A 2022, 10, 14051; El-Kady M., Kaner RBScalable fabrication of high-power graphene micro-supercapacitors for flexible and on-chip energy storage. Nat. Commun. 2013, 4, 1475-1483.].

[0003] With the development of wearable electronic devices, it is necessary not only to manufacture 2D SCs, but also to improve their energy density and stretchability to meet the needs of long-term continuous and stable operation of electronic devices. Electrode materials and electrode structures play a key role in the performance of 2D SCs. Designing new electrode materials with high conductivity and high specific surface area is the focus of improving the energy storage of 2D SCs [Zhang CF, Ma YL, Zhang XT, et al. Two-dimensional transition metalcarbides and nitrides (MXenes): synthesis, properties, and eElectr℃chemical energy storage applications. Energy Environ. Mater. 2020, 3, 29-5529.].

[0004] The energy storage properties of 2D SCs can be improved through the following strategies: 1) Hybridizing pseudocapacitive materials with graphene to form composite electrodes is an effective strategy for increasing energy density. Pseudocapacitive materials are redox active, while graphene is conductive. The resulting nanocomposites possess both excellent electrochemical activity and conductivity. 2) The preparation of asymmetric 2D SCs with a wider voltage output can also improve their energy density [Couly C., Alhabeb M., Aken KLV, et al. Asymmetric Flexible MXene-Reduced Graphene Oxide Micro-Supercapacitor. Adv. Electron. Mater. 2018, 4, 1700339.]. Strategies such as combining pseudocapacitive active materials with carbon materials to form hybrid materials or designing asymmetric 2D SCs can improve the specific capacitance and energy density of 2D SCs. However, the rigidity of pseudocapacitive materials such as PANI causes them to lose conductivity at low strains, severely limiting their application in stretchable electrodes. In this regard, pseudocapacitive materials such as PANI can be deposited or embedded on a polymer substrate with a stretchable structure to weaken its shortcomings. Special structural designs (such as serpentine, island bridge, wave, etc.) enable the device to exhibit good stretchability without being restricted by materials. When the electrode is stretched, the stretchable structure dissipates stress by stretching the curved segments, avoiding the shedding and cracking of the electrode material, thereby enhancing the tensile strain of the two-dimensional stretchable SCs. For example, when the wavy structure is stretched, the angle between the waves and the distance between the waves will increase to reduce the effect of external tension on the electrochemical performance of the device. This stretchable device obtained through structural design has the advantage of not being restricted by materials.

[0005] However, stretchable structures face a major challenge: their lack of resilience after stretching. Furthermore, most two-dimensional stretchable SCs require a substrate for support, making them suitable only for applications involving relatively small deformations, such as bending, folding, and twisting. Furthermore, when the substrate and electrode electrolyte deform out of sync during stretching, interfacial misalignment, delamination, and shedding can occur, leading to increased resistance and decreased performance.

[0006] Therefore, providing a novel structure to simultaneously meet the requirements of two-dimensional stretchable SCs with high stretchability, high energy and power density is a technical problem that needs to be urgently solved by technicians in this field. Summary of the Invention

[0007] In light of this, the present invention utilizes a bulk and interfacial synergistic energy dissipation strategy to develop a nested viscous multiphase gel based on a viscous electrolyte for the construction of a two-dimensional stretchable supercapacitor with ultrahigh strain, ultrahigh energy density, and ultrahigh power density. The present invention embeds semi-gel electrodes into the semi-gel viscous electrolyte through printing to form a nested viscous multiphase gel supercapacitor. This strategy utilizes a bulk and interfacial synergistic energy dissipation strategy to enhance the overall performance of two-dimensional supercapacitors (SCs), including stretchability and energy density.

[0008] The present invention's two-dimensional stretchable supercapacitor (nested viscous multiphase gel) based on a viscous electrolyte is formed by embedding a semi-gel electrode into a semi-gel viscous electrolyte by printing. The present invention names this composite viscous gel consisting of two parallel gel electrodes and a viscous gel electrolyte a viscous multiphase gel supercapacitor. The electrolyte viscous hydrogel is prepared from acrylamide (AM), 2-acrylamido-2-methylpropanesulfonic acid (AMPS), Irgacure 2959, N,N-methylenebisacetamide (MBA), polyvinyl alcohol (PVA), and phytic acid (PA) via a two-step free radical polymerization and freeze-thaw process. The electrode hydrogel, PVA / PA / PANI / PW-PMO, is prepared from heteropolyacid (HPA), polyvinyl alcohol, phytic acid, and polyaniline (PANI) via a two-step heating and freeze-thaw process (the preparation method of PVA / PA / PANI / PW-PMO can be found in the prior art patent No. CN117164892B).

[0009] To achieve the above object, the present invention adopts the following technical solutions:

[0010] A method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte comprises the following steps:

[0011] (1) Preparation of PAMS-m hydrogel electrolyte:

[0012] 1) Dissolving polyvinyl alcohol 1788 in phytic acid, adding sulfuric acid, and heating and stirring the mixture to obtain a PVA / PA solution;

[0013] 2) adding Irgacure 2959, N,N-methylenebisacetamide, acrylamide, and acrylamide-2-methylpropanesulfonic acid to the PVA / PA solution and stirring until the components are dissolved to obtain a hydrogel precursor;

[0014] 3) pouring the prepared hydrogel precursor solution into a mold to form a quasi-gel after ultraviolet light irradiation;

[0015] 4) Freezing and thawing the quasi-gel electrolyte to obtain a PAMS-m hydrogel electrolyte;

[0016] (2) Preparation of nested viscous multiphase gel of PVA / PA / PANI / PW-PMO@PAMS-m: PVA / PA / PANI / PW-PMO gel electrode quasi-gel was injected into the body of PAMS-m hydrogel electrolyte to form a nested viscous multiphase gel, which is a two-dimensional stretchable supercapacitor based on viscous electrolyte.

[0017] Furthermore, the PAMS-m hydrogel electrolyte in step (1) is prepared from the following raw materials in mass percentage: polyvinyl alcohol 1788 10.15% to 11.89%, phytic acid 69.84% to 71.59%, acrylamide-2-methylpropanesulfonic acid 1.24% to 2.23%, acrylamide 10.81% to 12.82%, Irgacure 2959 0.141% to 0.161%, and the balance is N,N-methylenebisacetamide.

[0018] Furthermore, the phytic acid is a phytic acid aqueous solution with a mass concentration of 50-70%.

[0019] Furthermore, in step 1), the heating and stirring temperature is 75° C. to 95° C., and the heating and stirring time is 2 to 4 hours.

[0020] Furthermore, in step 3), the wavelength of ultraviolet light irradiation is 365 nm, the intensity of ultraviolet light irradiation is 8 W, and the ultraviolet light irradiation time is 2 to 4 minutes.

[0021] Furthermore, the freeze-thaw method in step 4) is: freezing at -25°C to -30°C for 20 to 24 hours, and then thawing at room temperature for 1 to 2 hours.

[0022] Furthermore, the specific preparation method of step (2) PVA / PA / PANI / PW-PMO@PAMS-m nested viscous multiphase gel is as follows:

[0023] a) First, the PAMS-m hydrogel electrolyte is injected into the mold;

[0024] b) PVA / PA / PANI / PW-PMO quasi-gel was laid on the top of PAMS-m electrolyte quasi-gel to form two parallel electrodes with controllable gaps;

[0025] c) Adding PAMS-m quasi-gel to the upper layer of PVA / PA / PANI / PW-PMO quasi-gel to cover the mold, ensuring that the PVA / PA / PANI / PW-PMO gel electrode is completely integrated into the PAMS-m hydrogel electrolyte body;

[0026] d) The mold was freeze-thawed to form a nested viscous multiphase gel of PVA / PA / PANI / PW-PMO@PAMS-m.

[0027] Furthermore, the freeze-thaw method in step d) is: freezing at -25°C to -30°C for 20 to 24 hours, and then thawing at room temperature for 1 to 2 hours.

[0028] The beneficial effects of the present invention are as follows: the present invention proposes a strategy of coordinated energy dissipation of the bulk and interface to improve the comprehensive performance of supercapacitors (SCs), such as stretchability and energy density. To this end, a new type of viscous hydrogel with a multiple cross-linked network was designed and prepared using PVA, PA, 2-acrylamide-2-methylpropanesulfonic acid (AMPS) and acrylamide (AM) as substrates. The multiphase gel supercapacitor formed by printing the PVA / PA / PANI / PW-PMO gel electrode into the viscous hydrogel electrolyte has stronger interfacial adhesion. At the same time, the AMPS in the hydrogel contains highly dissociated sulfonic acid groups, which can greatly improve the proton conductivity of the gel electrolyte, thereby improving the energy density of the multiphase gel capacitor. The multiple cross-linked network formed by AM, AMPS, PVA and PA has high tensile properties. Secondly, simulation tests and comparative experiments were used to prove that the hydrogel electrolyte wrapped on the surface of the hydrogel electrode can effectively disperse stress and effectively protect the electrode. As the strain gradually increases, the stress gradually transfers to the interface, and the non-covalent fracture and recombination at the interface continue to dissipate the applied energy, further inhibiting the growth of macro cracks, thereby maintaining the integrity of the interface between the electrode and the electrolyte, and improving the tensile properties of the multiphase gel SCs. The advantage of this invention is that it utilizes the high proton conductivity of the gel electrolyte, the interfacial adhesion characteristics, and the wrapping structure of the nested viscous multiphase gel to achieve a tensile strain of 500%, 4122.0F cm -2 Capacitance, 5760.0 μW cm -2 High power density and 1319.0 μWh cm -2 high energy density. BRIEF DESCRIPTION OF THE DRAWINGS

[0029] Figure 1 This is a scanned image of the PAMS-1.8% viscous hydrogel in Example 1;

[0030] Figure 2 The stress-strain curves (a) of the PAMS-m hydrogel and (b) of the PVA / P(AM-AMPS)-n hydrogel in Example 1 are shown.

[0031] Figure 3 These are the tensile loading and unloading curves of the PAMS-1.8% hydrogel in Example 1.

[0032] Figure 4EIS curve of PAMS-1.8% hydrogel in Example 1 (a); conductivity of PAMS-1.8% hydrogel (b); proton conductivity of PAMS-1.8% at 25-38°C (c); Arrhenius plot of proton conductivity of PAMS-1.8% (d).

[0033] Figure 5 Pictures (a) to (d) of PAMS-1.8% hydrogel adhering to different substrates in Example 1; picture of the hydrogel during the peeling process; (e) peeling curve of PAMS-1.8% hydrogel; schematic diagram of the interface adhesion between PAMS-1.8% hydrogel and electrode (g).

[0034] Figure 6 This is a digital image of the PVA / PA / PANI / PW-PMO@PAMS-1.8% nested viscous multiphase gel in Example 1;

[0035] Figure 7 Optical microscope photographs of the PVA / PA / PANI / PW-PMO / / PAMS-1.8%~SCs interface under different tensile strains in Example 1: (a) 280%; (b) 600%; optical microscope photographs of the PVA / PA / PANI / PW-PMO@PAMS-1.8%SCs interface under different tensile strains: (c) 500%; (d) 900%.

[0036] Figure 8 This is the GCD of (a) to (e) wavy PVA / PA / PANI / PW-PMO@PAMS-1.8% to PVA / PA / PANI / PW-PMO@PAMS-3.6% in Example 1; (f) capacitance retention of wavy PVA / PA / PANI / PW-PMO@PAMS-1.8% to PVA / PA / PANI / PW-PMO@PAMS-3.6%.

[0037] Figure 9 (a) Neo-Hooke model of PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel in Example 1; (b) to (d) calculated images of the Neo-Hooke model of PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel under different forced displacements.

[0038] Figure 10 Calculation images of the Neo-Hooke model for (a) to (c) PAMS-1.8% electrolyte in Example 1 at different forced displacements; (d) to (f) calculation images of the Neo-Hooke model for PVA / PA / PANI / PW-PMO electrode at different forced displacements;

[0039] Figure 11 Electrochemical behaviors of PVA / PA / PANI / PW-PMO@PAMS-1.8% stretchable SCs in Example 1: (a) CV curve; (b) GCD curve; (c) Ragone curve; (d) Ragone plot of PVA / PA / PANI / PW-PMO@PAMS-1.8% SCs and PVA / PA / PANI / (PW-12%)-(PMO-12%)@PVA / SA / PA stretchable SCs; EIS curve of PVA / PA / PANI / PW-PMO@PAMS-1.8% stretchable SCs (e).

[0040] Figure 12 Electrochemical behavior of PVA / PA / PANI / PW-PMO@PAMS-1.8% stretchable SCs in Example 1: (a) CV curve; (b) GCD curve. DETAILED DESCRIPTION

[0041] The following will clearly and completely describe the technical solutions in the embodiments of the present invention in conjunction with the accompanying drawings. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without making creative efforts are within the scope of protection of the present invention.

[0042] Example 1

[0043] (1) Preparation of high-viscosity and high-proton-conductive PAMS-1.8% hydrogel:

[0044] PVA / PA / P(AM-AMPS)-1.8% (abbreviated as PAMS-1.8%) hydrogel electrolyte was prepared by photoinitiated free radical polymerization and freeze-thaw cycle method.

[0045] The specific preparation method of PAMS-1.8% gel is as follows:

[0046] 1) Dissolve 2.0 g of PVA in 10.0 mL of PA (50% water content), add 0.2 mL of SA, and stir the mixture at 95°C for 2 h to obtain a PVA / PA solution;

[0047] 2) Add 0.003 g Irgacure 2959, 0.00136 g MBA, 2.27 g AM, and 0.35 g AMPS to the above PVA / PA solution and stir vigorously until all ingredients are dissolved;

[0048] 3) Pour the prepared hydrogel precursor solution into a mold and place it under ultraviolet light (λ = 365 nm light, intensity 8 W) for 3 minutes to form a quasi-gel;

[0049] 4) The quasi-gel electrolyte was frozen at -30°C for 24 hours and thawed at room temperature for 2 hours to obtain a PAMS-1.8% hydrogel electrolyte.

[0050] Figure 1 This is a scanned image of PAMS-1.8% viscous hydrogel; from the image, it can be seen that PAMS-1.8% hydrogel forms a three-dimensional porous microstructure, and the porous network structure can effectively dissipate the stress applied to the hydrogel during the stretching process.

[0051] (2) Mechanical properties of PAMS-1.8% viscous hydrogel

[0052] Mechanical properties: The deformation and destruction characteristics of a material under the action of external forces are called mechanical properties of the material. The mechanical properties of a material are usually understood through testing. The most basic test is the axial tension and compression test of the material. The two ends of a PAMS-1.8% hydrogel with a length of 30 mm, a width of 8 mm and a thickness of 3 mm were fixed vertically on an electronic universal material testing machine and tested at a speed of 30 mm / min for 25 ℃ The material is stretched longitudinally at a temperature of 100°C, and the applied force (the additional internal force per unit area) and the resulting strain (when an object is deformed by force, the degree of deformation at different points in the body is generally not the same. A mechanical quantity used to describe the degree of deformation at a point) are recorded until it breaks. These two parameter data are then plotted on an XY graph to obtain the familiar stress-strain curve. The stress-strain curve is data that shows how stress changes with increasing strain. The slope of the stress-strain curve is used to obtain the Young's modulus to evaluate its strength.

[0053] The two ends of a PAMS-1.8% hydrogel with a length of 30 mm, a width of 8 mm and a thickness of 3 mm were fixed vertically on an electronic universal material testing machine and the loading (when the stress of the sample changes (0-800%), new plastic deformation occurs in the sample. This stress change is called loading) and unloading (when the stress changes, the sample returns to the initial state (800-0%) and no new plastic deformation occurs. At this time, the stress change is called unloading) curves of the PAMS-1.8% hydrogel were recorded with increasing strain (0-800%) at a speed of 30 mm / min and a fixed maximum strain of 800%. The area of ​​the loading and unloading curves is the area of ​​the hysteresis loop. The size of the area of ​​the hysteresis loop is used to evaluate its energy dissipation.

[0054] Figure 2 The mechanical properties of PAMS-1.8% viscous hydrogel electrolyte and PVA / P(AM-AMPS) hydrogel were evaluated. Figure 2 As shown in a, the tensile strength of the PAMS-1.8% hydrogel electrolyte is 372.3 kPa, and the elongation at break is 1596.0%. The fracture strength and strain of the PAMS-1.8% hydrogel (372.3 kPa and 1596.0%) are greater than those of the PVA / P(AM-AMPS) hydrogel without PA (196.8 kPa and 1134.0%). Figure 2 b), indicating that the addition of PA can form multiple hydrogen bonds with PVA, which alleviates the collapse of the network to a certain extent and enhances the mechanical properties of PAMS-1.8% hydrogel.

[0055] In order to study the fatigue properties of PAMS-1.8% hydrogel, tensile loading and unloading tests were performed. Figure 3 As shown in Figure 3, in the loading-unloading test, PAMS-1.8% hydrogel exhibited a relatively small hysteresis loop (hysteresis represents energy dissipation).

[0056] This result shows that: 1) PAMS-m hydrogel effectively dissipates external energy by destroying the cross-linked network during stretching; 2) The physical cross-linked network is dynamic and can recover even if it is destroyed under large deformation. To a certain extent, it is difficult to completely destroy the network of PAMS-m hydrogel. PAMS-1.8% hydrogel electrolyte exhibits high mechanical recovery ability under certain tensile strain; 3) The rich three-dimensional porous structure of PAMS-1.8% hydrogel promotes stress dissipation, and the unique network structure reduces hysteresis, making the hydrogel electrolyte more flexible.

[0057] (3) Proton conductivity of PAMS-1.8% viscous hydrogel

[0058] A PAMS-1.8% hydrogel electrolyte was coated in a polytetrafluoroethylene mold with specifications of 11 mm in length, 6 mm in width, and 2 mm in height. Its proton conductivity was measured using a Solarton 1260A AC impedance analyzer (AMETEK, USA). The two-probe method was used for testing, with a perturbation voltage of 10 mV and a test frequency of 0.1 Hz to 100 kHz. The conductivity was then calculated using the formula K = L / RS, where L is the distance between the two probes, S is the cross-sectional area of ​​the viscous hydrogel (i.e., the product of the width and thickness of the viscous hydrogel), and R is the resistance of the viscous hydrogel. Three measurements were taken and the average was taken to obtain the final proton conductivity value.

[0059] Figure 4The proton conductivity of PAMS-1.8% hydrogel is evaluated. The sulfonic acid groups on the AMPS molecules are ionized in water to produce freely movable ions. These ions "transition" in the molecular chain to achieve ion transport. Therefore, the introduction of AMPS into the hydrogel can make the hydrogel have good proton conductivity. As shown in 4a, b, at 25 ℃ The proton conductivity of PAMS-1.8% hydrogel electrolyte is 0.07 under constant humidity conditions. Under constant humidity conditions at 38℃, the proton conductivity of PAMS-1.8% ( Figure 4 c) are 0.126S cm -1 (m=1.8%), which is improved. According to the Arrhenius formula, it can be concluded that the activation energy of PAMS-1.8% is around 0.12eV ( Figure 4 d), consistent with the Grothuss proton conduction mechanism.

[0060] (4) Adhesion properties of PAMS-1.8% adhesive hydrogel

[0061] 90° Peel Test: Wipe a 50x127x1.6mm stainless steel test panel with a clean cloth / paper wipe dampened with isopropyl alcohol or denatured alcohol. Allow to dry, ensuring there is no visible contamination on the surface. Using a blade and cutting tool, cut the tape sample into 25.4mm x 115mm strips to be tested. Ensure the strip length aligns with the tape winding direction. Lay the cut sample onto the cleaned stainless steel test panel. Remove the release film. Lift the other end of the tape and gradually press it with a 2kg rubber roller to avoid air bubbles and wrinkles. Allow the laminated adhesive hydrogel to rest at room temperature (23±2°C, 55%±10%) for 20-30 minutes. Peel a section of tape (approximately 10-20mm) from one end of the test panel for clamping, with the peeled end facing outward. Secure the stainless steel panel to the 90° test platform, adjust the upper fixture to its initial position, and zero the test. Hold the peeled section of the tape at a 90° angle to the surface and secure it with the upper clamp. Set the peel tester speed to 300 mm / min. Start the tester and begin peeling the tape at the set speed. During the peeling process, the tester records the peel force and peel distance data, and the effective peel curve is displayed on the computer. After the test is completed, record the maximum peel force (unit: N) and the average peel distance (unit: m) during the peeling process to determine the adhesion properties of the hydrogel.

[0062] Figure 5 The purpose is to evaluate the adhesion performance of PAMS-1.8% viscous hydrogel electrolyte. Figure 5As shown in a to d, PAMS-1.8% hydrogel electrolyte can adhere to different materials, such as polypropylene (PP), polyetheretherketone (PEEK), polycarbonate (PC), peptide (Ti), glass, quartz and shell. The 90° peeling test further proves the adhesion performance of PAMS-1.8% hydrogel electrolyte. Figure 5 As shown in e and f, the interfacial toughness of PAMS-1.8% hydrogel electrolyte is: PAMS-1.8%: 270.26 J / m 2 Since the sulfonic acid groups on the AMPS molecules form electrostatic interactions with the PANI in the PVA / PA / PANI / PW-PMO electrode, and the two carbonyl groups on the sulfonic acid groups have stronger proton-accepting abilities than pure hydroxyl groups, they are more likely to form hydrogen bonds with the PVA / PA / PANI / PW-PMO ( Figure 5 g), therefore, the interfacial toughness between the PAMS-1.8% hydrogel electrolyte and the electrode is greater than that between the PVA / PA hydrogel electrolyte and the electrode.

[0063] (5) Preparation of PVA / PA / PANI / PW-PMO@PAMS-1.8% Nested Viscous Multiphase Gel

[0064] Inject PVA / PA / PANI / PW-PMO (preparation method can be found in the prior art CN117164892B) gel electrode quasi-gel into the body of PAMS-1.8% quasi-gel to form a nested viscous multiphase gel:

[0065] 1) First, inject PAMS-1.8% quasi-gel electrolyte into the mold;

[0066] 2) PVA / PA / PANI / PW-PMO quasi-gel was injected into the PAMS-1.8% electrolyte quasi-gel to form two parallel electrodes with controllable gaps;

[0067] 3) Add PAMS-1.8% quasi-gel to the top layer to cover the mold, ensuring that the PVA / PA / PANI / PW-PMO gel electrode is completely integrated into the PAMS-1.8% quasi-gel electrolyte body;

[0068] 4) The mold was frozen at -25°C to -30°C for 20 to 24 hours and then thawed at room temperature for 1 to 2 hours to form a PVA / PA / PANI / PW-PMO@PAMS-1.8% nested viscous multiphase gel.

[0069] Figure 6This is a digital photo of the nested viscous multiphase gel of PVA / PA / PANI / PW-PMO@PAMS-1.8%. It can be seen from the picture that the PAMS-1.8% electrolyte surrounds the PVA / PA / PANI / PW-PMO electrode, explaining the structure of its multiphase gel.

[0070] (6) Energy dissipation mechanism of PVA / PA / PANI / HPA@PAMS-1.8% nested viscous multiphase gel supercapacitor during stretching

[0071] Comparative experiment: In order to explore the interfacial energy dissipation mechanism of PVA / PA / PANI / PW-PMO@PAMS-1.8% during the stretching process, multiphase gel stretchable SCs with different viscosities were constructed and their tensile properties were evaluated respectively.

[0072] Interface conditions of multiphase gel supercapacitors under stretching: The freeze-dried PVA / PA / PANI / PW-PMO@PAMS-1.8% nested viscous multiphase gel (30 mm long, 8 mm wide, 3 mm thick) was bonded to the cross-section stage (30 mm in diameter) used for scanning electron microscopy, and the fusion of the electrode and electrolyte interface regions in the multiphase gel was detected under the scanning electron microscope (for example, whether there is a seamless connection in the interface region); the PVA / PA / PANI / PW-PMO@PAMS-1.8% nested viscous multiphase gel (30 mm long, 8 mm wide, 3 mm thick) and the sandwich-type supercapacitor (30 mm long, 8 mm wide, 3 mm thick) were placed under a microscope, and the changes in the electrode and electrolyte interface regions (for example, whether there is stratification, cracking, etc. in the interface region) were observed under different stretching ratios (0% to 800%) [stretching ratio = (length after stretching - original length) / original length].

[0073] Simulating the interface of multiphase gel supercapacitors under tensile state: According to the stress-strain curves of PVA / PA / PANI / PW-PMO electrode, PAMS-1.8% electrolyte and PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel ( Figure 2a), it can be seen that the PVA / PA / PANI / PW-PMO electrode, PAMS-1.8% electrolyte and PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel is a large deformation, elastic and nonlinear material, which is considered to be a hyperelastic material in mechanics, and the Neo-Hooke model hyperelastic material has good convergence. According to the model requirements, a Neo-Hooke model of a PAMS-1.8% electrolyte hyperelastic material wrapped in another PVA / PA / PANI / PW-PMO electrode hyperelastic material, namely PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel, was established and uniaxially stretched. Then, the left end face of the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel model was constrained by uniaxial stretching, and the right end face was stretched by forced displacement (the model length was 10 mm, and the corresponding forced displacement was 30 mm), so as to simulate and determine when the PVA / PA / PANI / PW-PMO electrode and electrolyte material would separate. Based on the stress-strain data of the PVA / PA / PANI / PW-PMO electrode and PAMS-1.8% electrolyte, Abaqus simulations were used to determine the hyperelastic material parameters of the PVA / PA / PANI / PW-PMO electrode and PAMS-1.8% electrolyte. The separation criterion for the PVA / PA / PANI / PW-PMO electrode and PAMS-1.8% electrolyte is when one of the two materials reaches its ultimate fracture stress. During stretching, the material's fracture behavior is observed to determine the stress and energy dissipation.

[0074] Figure 7 This is a scanning electron micrograph of the fusion of the electrode and electrolyte interface regions in the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel (e.g., whether there is a seamless connection in the interface region). Figure 7 a, c); and microscopic digital photos of the changes in the electrode and electrolyte interface regions of the multiphase gel and sandwich gel PVA / PA / PANI / PW-PMO / / PAMS-1.8% at stretching ratios of 0% to 900% (e.g., whether there is delamination or cracking in the interface region, etc.) ( Figure 7 b, d); fluorescence microscopy ( Figure 7 a) shows that when the stretching ratio of PVA / PA / PANI / PW-PMO / / PAMS-1.8% is 280%, there is no obvious delamination or displacement at the interface between the electrode and the electrolyte. When the stretching ratio exceeds 600% ( Figure 7 b), electrode cracks become apparent, eventually leading to interface delamination and displacement. Figure 7As shown in Figures c and d, fluorescence microscopy shows that the PVA / PA / PANI / PW-PMO@PAMS-1.8% interface remains intact when the tensile strain exceeds 500%. When the tensile strain increases to 900%, the stress is transferred to the electrode-electrolyte interface. No cracking of the electrode-electrolyte interface was observed during the stretching process, indicating that the PVA / PA / PANI / PW-PMO@PAMS-1.8% wrapping structure and the adhesion properties of the electrode-electrolyte interface effectively maintain a close connection between the electrode and electrolyte interfaces.

[0075] Figure 8 In order to investigate the interfacial energy dissipation mechanism of PVA / PA / PANI / PW-PMO@PAMS-1.8% during stretching, multiphase gel stretchable SCs with different viscosities were constructed (denoted as PVA / PA / PANI / PW-PMO@PAMS-0.0%, PVA / PA / PANI / PW-PMO@PAMS-0.9%, PVA / PA / PANI / PW-PMO@PAMS-1.8%, PVA / PA / PANI / PW-PMO@PAMS-2.7% and PVA / PA / PANI / PW-PMO@PAMS-3.6%). Figure 8 As shown in Figures a-f, the capacitance retention of PVA / PA / PANI / PW-PMO@PAMS-0.0% SCs reaches 88% at a tensile strain of 350%. The capacitance retention of PVA / PA / PANI / PW-PMO@PAMS-0.9% SCs reaches 87% at a tensile strain of 420%. The capacitance retention of PVA / PA / PANI / PW-PMO@PAMS-1.8% SCs reaches 90% at a tensile strain of 500%. The capacitance retention of PVA / PA / PANI / PW-PMO@PAMS-2.7% SCs reaches 90% at a tensile strain of 450%. The capacitance retention of PVA / PA / PANI / PW-PMO@PAMS-3.6% SCs reaches 91% at a tensile strain of 320%. It can be seen that the tensile performance of supercapacitors increases with increasing electrolyte viscosity.

[0076] According to the stress-strain curves of PVA / PA / PANI / PW-PMO electrode, PAMS-1.8% electrolyte and PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel, it can be seen that PVA / PA / PANI / PW-PMO electrode, PAMS-1.8% electrolyte and PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel are large deformation, elastic and nonlinear materials. In mechanics, they are considered as hyperelastic materials, and the Neo-Hooke model hyperelastic material has good convergence. According to the model requirements, a Neo-Hooke model ( Figure 9 a) and subjected it to uniaxial stretching. The left end face of the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel model was then constrained to uniaxial stretching, while the right end face was stretched by forced displacement (the model length was 10 mm, corresponding to a forced displacement of 30 mm). This allowed simulation to determine when the PVA / PA / PANI / PW-PMO electrode and the electrolyte material would separate. Based on the stress-strain data of the PVA / PA / PANI / PW-PMO electrode and the PAMS-1.8% electrolyte, the hyperelastic material parameters of the PVA / PA / PANI / PW-PMO electrode and the PAMS-1.8% electrolyte were simulated in Abaqus software. The criterion for separation between the PVA / PA / PANI / PW-PMO electrode and the PAMS-1.8% electrolyte is when one of the materials reaches its ultimate fracture stress. From the simulation results 9b and c, it can be seen that when the right end face of the reinforced displacement moves by 30×0.05mm and 30×0.1438mm, that is, by 1.5mm and 4.314mm respectively, the degree of deformation of the electrolyte material continues to increase, and the maximum stress is 144.8kPa at this time. Figure 9 As shown in Figure d, when the right end face of the enhanced displacement moved 30 × 0.2246 mm, or 6.738 mm, the electrolyte material reached a fracture stress of approximately 281.2 kPa, causing the electrolyte to fracture. The Mises stress data indicate that the PVA / PA / PANI / PW-PMO electrode did not reach the fracture stress during the stretching process, and therefore did not fracture.

[0077] In order to further understand the deformation of PVA / PA / PANI / PW-PMO@PAMS-1.8% when stretching, we simulated them separately under the same conditions. Figure 10 As can be seen, the deformation of the electrolyte is largely consistent with that of the multiphase gel, with stress primarily concentrated in the electrolyte. These results suggest that during stretching, the PVA / PA / PANI / PW-PMO electrode undergoes minimal deformation, while the electrolyte dissipates energy through the rupture of non-covalent bonds, significantly protecting the PVA / PA / PANI / PW-PMO electrode. This suggests a mechanism for energy dissipation in the multiphase gel structure during stretching. During stretching, the low-modulus PAMS-1.8% hydrogel electrolyte encapsulating the electrode surface dissipates the energy during stretching. Furthermore, the encapsulated structure of the multiphase gel significantly increases the effective contact area between the electrode and electrolyte, facilitating stress transfer and dissipation within a fully connected and extended network. Secondly, as strain increases, the viscous interface formed by the viscous electrolyte dissipates the applied energy during separation through the rupture and recombination of non-covalent bonds, such as electrostatic and hydrogen bonds. This suppresses macroscopic crack growth, maintaining the integrity of the electrode-electrolyte interface and improving the tensile properties of the SC.

[0078] (7) Electrochemical Performance of PVA / PA / PANI / PW-PMO@PAMS-1.8% Nested Viscous Multiphase Gel Supercapacitors

[0079] The preparation method of nested viscous multiphase gel can refer to the prior art CN117164892B. This composite viscous gel composed of two parallel gel electrodes (PVA / PA / PANI / PW-PMO) embedded in the bulk phase of a viscous gel electrolyte (PAMS-1.8%) is named a viscous multiphase gel supercapacitor. Cyclic voltammetry (CV) curves of the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel stretchable supercapacitor were tested at 10-100mV / s using a Chenhua electrochemical workstation to evaluate the rate performance of the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel stretchable supercapacitor; based on the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel stretchable supercapacitor at 0.4-2.0mAcm -2The capacitance, energy density and power density of the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel stretchable supercapacitor were evaluated by galvanostatic charge-discharge (GCD) curves under different current densities. The electrochemical impedance spectroscopy (EIS) test was performed on the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel stretchable supercapacitor to evaluate the conductivity and diffusion behavior of its electrodes. Subsequently, the capacitance retention was determined by CV and GCD analysis of the PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel stretchable supercapacitor at different stretching ratios (0% to 500%). The CV and GCD tests at different stretching ratios of the capacitors obtained in series were performed to evaluate the performance of the flexible stretchable capacitors obtained in series.

[0080] Figure 11 The PVA / PA / PANI / PW-PMO semi-gel electrode is injected into the PAMS-1.8% semi-gel electrolyte to form a multiphase gel flexible stretchable supercapacitor. Figure 11 a It can be seen that at different current densities (0.4, 0.6, 0.8, 1.0 and 2.0 mA cm -2 ), the CV curve shows nonlinear characteristics, indicating that the capacitance behavior of the electrode is dominated by pseudocapacitance. According to the GCD curve ( Figure 11 b) shows that the current density is 0.4, 0.6, 0.8, 1.0 and 2.0 mA cm -2 When the capacitance (Cs) of PVA / PA / PANI / PW-PMO@PAMS-1.8% SC is 4122.0, 2598.4, 1762.0, 1490.0 and 1450.0 Fcm, respectively. -2 When the power density is 1158.0 μW cm -2 The maximum energy density of PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel can reach 1319.0 μWh cm -2 Even at the maximum power density of 5760.0 μW cm -2 When the energy density is maintained at 464.0 μWh cm -2 ( Figure 11 c). This result is much higher than the energy density of PVA / PA / PANI / PW-PMO@PAMS-1.8% SCs (see Chinese patent: CN117164892B). Figure 11 d), indicating that the excellent high proton conductivity of PAMS-1.8% hydrogel electrolyte can accelerate the reaction rate between the electrode and the electrolyte, thereby improving the performance of SCs. Figure 11 e) The internal resistance of the multiphase gel stretchable SCs is 10.33Ω, indicating the low interfacial resistance and fast and efficient kinetic process of the multiphase gel stretchable SCs.

[0081] Figure 12 The electrochemical performance of wavy PVA / PA / PANI / PW-PMO@PAMS-1.8% multiphase gel SCs under high strain was studied. Figure 12 As shown in Figures 12a and 12b, when the strain exceeds 500%, the CV and GCD curves remain basically unchanged, and the capacitance retention rate of PVA / PA / PANI / PW-PMO@PAMS-1.8% SCs is 90%.

[0082] In order to distinguish the advantages of the solution of the present invention compared with the existing technology, the following comparative experiments were conducted:

[0083] Comparative Example 1

[0084] Compared with the performance of the solution in patent CN117164892B: 1) Based on patent CN117164892B, a new strategy of synergistic energy dissipation between bulk and interface is further proposed. The gel electrode is placed in a high-viscosity, high-proton-conductive hydrogel electrolyte. By introducing a high-viscosity, high-proton-conductive gel electrolyte, the synergistic mechanism of interface energy dissipation and bulk energy dissipation is simultaneously adopted to further improve the comprehensive performance of the two-dimensional stretchable supercapacitor, such as stretchability, surface capacitance, and energy density. Compared with the bulk phase strategy used alone to improve supercapacitor performance in patent CN117164892B, the stretchability of the integrated multiphase gel SCs prepared by the present invention using the synergistic energy dissipation strategy of bulk and interface is increased to more than 500%, which is 1.5 times that of the SCs with single bulk phase energy dissipation in the previous patent CN117164892B. Under a tensile strain of 500%, the capacitance retention of the integrated multiphase gel SCs can reach over 90.0%. Under a tensile strain of 420%, after 3500 repeated stretching-release cycles, the capacitance retention remains over 96.0%. The specific capacitance of the multiphase gel SCs is as high as 4122.0 F cm -2 , with an energy density of up to 1319.0 μWh cm -2 , its area-specific capacitance and energy density are both six times greater than those of the stretchable multiphase gel SCs described in the previous patent CN117164892B. 2) While CN117164892B does not explore the stretching mechanism of the multiphase gel, the present invention uses simulations and comparative experiments to specifically investigate the bulk energy dissipation mechanism during stretching of the multiphase gel.

[0085] Comparative Example 2

[0086] Compared with Example 1, AM is not added, but only AM is added. As a comparative experiment, AM, Irgacure 2959, N,N-methylenebisacetamide (MBA), polyvinyl alcohol (PVA), and phytic acid (PA) were selected to prepare a viscous electrolyte through a two-step process of free radical polymerization and freeze-thaw. Compared with the electrolyte (PVA / PA) in patent CN117164892B, the multiple cross-linked networks formed by AM, PVA, and PA break first during the stretching process, dissipating energy to relieve stress concentration in the hydrogel and hindering the expansion of cracks, thereby protecting the other flexible network, allowing the hydrogel electrolyte structure to remain intact and improving its tensile properties. The electrolyte has a tensile property of 1500%, which is about twice that of the invention patent CN117164892B.

[0087] Comparative Example 3

[0088] Compared with Example 1, no AM is added, and only AMPS is added. As a comparative experiment, components including AMPS, Irgacure 2959, MBA, PVA and PA were selected to prepare a viscous electrolyte through free radical polymerization and freeze-thaw two-step method. Compared with the electrolyte (PVA / PA) in patent CN117164892B, the AMPS in the present invention is a compound containing sulfonic acid groups. The sulfonic acid groups are easily ionized in water to produce freely mobile ions. These ions "transition" in the molecular chain to achieve ion transport and have excellent proton conductivity, so that the proton conductivity of the electrolyte of the present invention reaches 5.0Sm -1 At the same time, a large number of sulfonic acid groups can undergo a variety of non-covalent interactions, such as dipole-dipole interaction and electrostatics, which endow the hydrogel with good wet adhesion properties, making the electrolyte of the present invention have excellent adhesion properties (270.26 J / m 2 ).

[0089] Comparative Examples 2-3 demonstrate that the addition of AM and AMPS can improve the stretchability, proton conductivity, and adhesion properties of the hydrogel. Furthermore, the reversible interfacial adhesion, high proton conductivity, and multiphase gel wrapping structure of the hydrogel electrolyte can significantly enhance the energy density, stretchability, and other properties of the two-dimensional stretchable supercapacitor. This result demonstrates that the use of AM and AMPS as the molecularly constructed electrolyte plays a crucial role in the present invention's strategy of synergistic bulk and interfacial energy dissipation to enhance the stretchability and energy density of two-dimensional supercapacitors; both are essential.

[0090] The results show that the present invention uses PVA, PA, 2-acrylamide-2-methylpropanesulfonic acid (AMPS) and acrylamide (AM) as substrates to prepare a type of viscous hydrogel with a multiple cross-linked network. The nested viscous multiphase gel supercapacitor formed by printing the PVA / PA / PANI / PW-PMO gel electrode into the viscous hydrogel electrolyte has stronger interfacial adhesion. At the same time, the AMPS in the hydrogel contains highly dissociated sulfonic acid groups, which can greatly improve the proton conductivity of the gel electrolyte, thereby improving the energy density of the nested viscous multiphase gel capacitor. The multiple cross-linked network formed by AM, AMPS, PVA and PA has ultra-high tensile properties. The AMPS in the hydrogel electrolyte contains a large number of active groups (sulfonic acid groups, hydroxyl groups, etc.) with good adhesion properties, and the sulfonic acid groups it contains can form a continuous hydrogen bond network with water molecules, with excellent proton conductivity, which is beneficial to proton transfer between the electrode and the electrolyte. The hydrogel electrolyte wrapped on the surface of the hydrogel electrode in the nested viscous multiphase gel constructed by the present invention can effectively disperse stress and effectively protect the electrode. As strain gradually increases, stress gradually transfers to the interface, where non-covalent fracture and recombination continue to dissipate applied energy, further suppressing the growth of macroscopic cracks, thereby maintaining the integrity of the electrode-electrolyte interface. The advantage of this invention lies in leveraging the electrolyte's high proton conductivity and adhesion properties, as well as the multiphase gel wrapping structure design, to give the prepared two-dimensional supercapacitor a comprehensive performance of ultra-high stretchability, area-specific capacitance, and energy density.

[0091] Example 2

[0092] The scheme is basically the same as that of Example 1. Other conditions remain unchanged. 2.27g AM and 0.35g AMPS are replaced with 2.62g AM and 0g AMPS. Then, PAMS-0.0% viscous hydrogel is prepared. Its tensile properties (2400%), proton conductivity (0.02S cm -1 ), adhesion performance (59.06J / m 2 ). According to the operating steps of Example 1, the PVA / PA / PANI / PW-PMO semi-gel was injected into the PAMS-0.0% viscous semi-gel stretchable electrolyte to form a nested multiphase gel and then assembled into a two-dimensional stretchable supercapacitor. Then the capacitance performance (3522.0F cm -2 ), energy density (1219.0 μWh cm -2 The above results show that the two-dimensional supercapacitors prepared by the strategy of bulk and interface synergistic energy dissipation have excellent electrochemical performance.

[0093] Example 3:

[0094] The method is basically the same as that of Example 1. Other conditions remain unchanged. 2.27g AM and 0.35g AMPS are replaced with 0.32g AM and 0.3g AMPS to prepare PAMS-0.9% viscous hydrogel. The tensile properties (2100%) and proton conductivity (0.04S cm -1 ), adhesion performance (122.49J / m 2 According to the operating steps of Example 1, the PVA / PA / PANI / PW-PMO semi-gel was injected into the PAMS-0.9% viscous semi-gel stretchable electrolyte to form a nested multiphase gel and then assembled into a two-dimensional stretchable supercapacitor. The capacitance performance (3562.0F cm -2 ), energy density (1259.0 μWh cm -2 The above results show that the two-dimensional supercapacitors prepared by the bulk and interface synergistic energy dissipation strategy have excellent electrochemical performance.

[0095] Example 4

[0096] The method is basically the same as that of Example 1. Other conditions remain unchanged. 2.27g AM and 0.35g AMPS are replaced with 2.22g AM and 0.40g AMPS to prepare PAMS-2.7% viscous hydrogel. The tensile properties (1350%) and proton conductivity (0.075S cm -1 ), adhesion performance (185.34J / m 2 According to the operating steps of Example 1, the PVA / PA / PANI / PW-PMO semi-gel was injected into the PAMS-2.7% viscous semi-gel stretchable electrolyte to form a nested multiphase gel and then assembled into a two-dimensional stretchable supercapacitor. The capacitance performance (4142.0F cm -2 ), energy density (1339.0 μWh cm -2 The above results show that the two-dimensional supercapacitors prepared by the strategy of synergistic energy dissipation between bulk and interface have excellent electrochemical performance.

[0097] Example 5

[0098] The method is basically the same as that of Example 1. Other conditions remain unchanged. 2.27g AM and 0.35g AMPS are replaced with 2.17g AM and 0.45g AMPS to prepare PAMS-3.6% viscous hydrogel. The tensile properties (1020%) and proton conductivity (0.079S cm -1 ), adhesion performance (177.59J / m 2). According to the operating steps of Example 1, the PVA / PA / PANI / PW-PMO semi-gel was injected into the PAMS-3.6% viscous semi-gel stretchable electrolyte to form a nested multiphase gel and then assembled into a two-dimensional stretchable supercapacitor. Then the capacitance performance (4152.0F cm -2 ), energy density (1349.0 μWh cm -2 The above results show that the two-dimensional supercapacitors prepared by the strategy of bulk and interface synergistic energy dissipation have excellent electrochemical performance.

[0099] Although the embodiments of the present invention have been shown and described above, it will be understood that the above embodiments are illustrative and are not to be construed as limitations on the present invention. A person skilled in the art may change, modify, replace and modify the above embodiments within the scope of the present invention.

Claims

1. A method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte, characterized in that: The following steps are involved: (1) Preparation of PAMS-m hydrogel electrolyte: 1) Dissolving polyvinyl alcohol 1788 in phytic acid, adding sulfuric acid, and heating and stirring the mixture to obtain a PVA / PA solution; 2) adding Irgacure 2959, N,N-methylenebisacetamide, acrylamide, and acrylamide-2-methylpropanesulfonic acid to the PVA / PA solution and stirring until the components are dissolved to obtain a hydrogel precursor; 3) Pour the prepared hydrogel precursor solution into a mold and form a quasi-gel after UV irradiation for a few minutes; 4) Freezing and thawing the quasi-gel electrolyte to obtain the PAMS-m hydrogel electrolyte; (2) Preparation of nested viscous multiphase gel of PVA / PA / PANI / PW-PMO@PAMS-m: PVA / PA / PANI / PW-PMO gel electrode quasi-gel was injected into the body of PAMS-m hydrogel electrolyte to form a nested viscous multiphase gel, which is a two-dimensional stretchable supercapacitor based on viscous electrolyte.

2. The method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte according to claim 1, characterized in that: The PAMS-m hydrogel electrolyte in step (1) is prepared from the following raw materials in mass percentage: polyvinyl alcohol 1788 10.15% to 11.89%, phytic acid 69.84% to 71.59%, acrylamide-2-methylpropanesulfonic acid 1.24% to 2.23%, acrylamide 10.81% to 12.82%, Irgacure 2959 0.141% to 0.161%, and the balance is N,N-methylenebisacetamide.

3. The method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte according to claim 1, characterized in that: In step 1), the heating and stirring temperature is 75° C. to 95° C., and the heating and stirring time is 2 to 4 hours.

4. The method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte according to claim 1, characterized in that: In step 3), the wavelength of ultraviolet light irradiation is 365 nm, the intensity of ultraviolet light irradiation is 8 W, and the ultraviolet light irradiation time is 2 to 4 minutes.

5. The method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte according to claim 1, characterized in that: The freeze-thaw method in step 4) is: freezing at -25°C to -30°C for 20 to 24 hours, and then thawing at room temperature for 1 to 2 hours.

6. The method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte according to claim 1, characterized in that: The specific preparation method of step (2) PVA / PA / PANI / PW-PMO@PAMS-m nested viscous multiphase gel is as follows: a) First, the PAMS-m hydrogel electrolyte is injected into the mold; b) PVA / PA / PANI / PW-PMO quasi-gel was laid on the top of PAMS-m electrolyte quasi-gel to form two parallel electrodes with controllable gaps; c) Adding PAMS-m quasi-gel to the upper layer of PVA / PA / PANI / PW-PMO quasi-gel to cover the mold, ensuring that the PVA / PA / PANI / PW-PMO gel electrode is completely integrated into the PAMS-m hydrogel electrolyte body; d) The mold was freeze-thawed to form a nested viscous multiphase gel of PVA / PA / PANI / PW-PMO@PAMS-m.

7. The method for preparing a two-dimensional stretchable supercapacitor based on a viscous electrolyte according to claim 1, characterized in that: The freeze-thaw method in step d) is: freezing at -25°C to -30°C for 20 to 24 hours, and then thawing at room temperature for 1 to 2 hours.

8. A two-dimensional stretchable supercapacitor based on a viscous electrolyte, characterized in that: The method according to any one of claims 1 to 7 is used to prepare the present invention.

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