CN109687040A - Compressible rechargeable zinc-manganese battery and battery-sensor integrated device based on same - Google Patents
Compressible rechargeable zinc-manganese battery and battery-sensor integrated device based on same Download PDFInfo
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- CN109687040A CN109687040A CN201811571696.8A CN201811571696A CN109687040A CN 109687040 A CN109687040 A CN 109687040A CN 201811571696 A CN201811571696 A CN 201811571696A CN 109687040 A CN109687040 A CN 109687040A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/36—Accumulators not provided for in groups H01M10/05-H01M10/34
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention discloses a compressible rechargeable zinc-manganese battery and a battery-sensor integrated device based on the same, which comprises a positive electrode, a negative electrode and an electrolyte, wherein the negative electrode adopts an active material taking zinc as a main element, and the positive electrode active material is manganese dioxide; the electrolyte is a crosslinked polyacrylamide hydrogel electrolyte, and the synthesis method of the crosslinked polyacrylamide hydrogel electrolyte comprises the following steps: adding 3-5 g of monomer acrylamide, 25-35 mg of ammonium persulfate initiator and 3-5 mg of N' N-dimethyl bisacrylamide into 15-25 ml of deionized water, and continuously stirring until the mixture is clear; then transferring the clear solution into a glass surface vessel, coating the glass surface vessel with tinfoil paper, and reacting at 50-70 ℃ for 50-70 min to obtain hydrogel; finally, the hydrogel is placed in 0.8-1.2 mol/L zinc sulfate and 0.05-0.15 mol/L manganese sulfate electrolyte for full soaking, and the cross-linked polyacrylamide hydrogel electrolyte is obtained. The battery can adapt to larger compressive stress and simultaneously can keep energy storage performance, and the flexibility and the elasticity of energy storage equipment can be realized.
Description
Technical Field
The invention relates to a compressible rechargeable zinc-manganese battery and a battery-sensor integrated device based on the compressible rechargeable zinc-manganese battery.
Background
In order to realize the power supply for the flexible wearable electronic device, the design and development of a flexible energy storage device become one of the directions of the research of the novel energy storage device at the present stage. However, it is difficult to design an elastic energy storage device on the basis of the three-layer structure of electrode/membrane/electrode of the conventional energy storage device. Therefore, new technical paths are needed to achieve the flexibility and elasticity of the energy storage device.
Currently, some advances have been made in stretchable energy storage devices, such as stretchable supercapacitors or stretchable batteries, based on stretchable electrodes or hydrogel electrolytes. However, the research progress of the compressible energy storage device is still very limited, and in order to supply power to the corresponding compressible electronic device, such as the compressible pressure sensor, it is one of the issues to be solved urgently to develop an energy storage device capable of accommodating a large compressive stress while maintaining the energy storage performance.
Disclosure of Invention
The invention aims to solve the technical problems and provides a compressible rechargeable zinc-manganese battery and a battery-sensor integrated device based on the compressible rechargeable zinc-manganese battery, wherein the battery can adapt to larger compressive stress and maintain energy storage performance, and the flexibility and the elasticity of energy storage equipment can be realized.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a compressible rechargeable zinc-manganese battery comprises a positive electrode, a negative electrode and an electrolyte containing anions and cations and having ionic conductivity, wherein the negative electrode adopts an active material taking zinc as a main element, and the positive electrode active material is manganese dioxide; the electrolyte is a crosslinked polyacrylamide hydrogel electrolyte, and the synthesis method of the crosslinked polyacrylamide hydrogel electrolyte comprises the following steps: adding 3-5 g of monomer acrylamide, 25-35 mg of ammonium persulfate initiator and 3-5 mg of N' N-dimethyl bisacrylamide into 15-25 ml of deionized water, and continuously stirring until the mixture is clear; then transferring the clear solution into a glass surface vessel, coating the glass surface vessel with tinfoil paper, and reacting at 50-70 ℃ for 50-70 min to obtain hydrogel; finally, the hydrogel is placed in 0.8-1.2 mol/L zinc sulfate and 0.05-0.15 mol/L manganese sulfate electrolyte for full soaking, and the cross-linked polyacrylamide hydrogel electrolyte is obtained.
Specifically, the negative electrode material is prepared by electrodeposition of graphite paper serving as a current collector under a three-electrode system by a potentiostatic method of-1.3 to-1.5V.
Specifically, the electrolyte used in the electrodeposition process contains 0.1-0.3 mol/L of zinc sulfate and 0.4-0.6 mol/L of sodium citrate.
Specifically, the positive electrode active material manganese dioxide is prepared by a hydrothermal method.
More specifically, the hydrothermal method for preparing manganese dioxide comprises the following steps: fully mixing 0.02-0.04 mol of manganese sulfate, 1-3 ml of 0.4-0.6 mol/L sulfuric acid, 80-100 ml of deionized water and 15-25ml of 0.0.05-0.15 mol/L potassium permanganate at room temperature to obtain a mixed solution; then transferring the mixed solution to hot compress with water and reacting for 10-14 h at 100-140 ℃; then washing the hydrothermal product with deionized water to be neutral and drying in vacuum to obtain dried manganese oxide; mixing the dried manganese oxide, a conductive agent and a binder in N' -methyl pyrrolidone according to the proportion of 7.
As a preferable scheme, the conductive agent is acetylene black; the binder is polyvinylidene fluoride.
The invention also provides a battery-sensor integrated device, and the battery is integrated with the pressure sensor.
Compared with the prior art, the invention has the following beneficial effects:
(1) The invention develops and uses a chemically cross-linked polyacrylamide hydrogel as an electrolyte of a rechargeable zinc ion battery in order to improve the compressibility of the battery. Compared with the common battery diaphragm, the polyacrylamide hydrogel has good water retention performance and is compatible with ions in zinc ion electrolyte. Therefore, the hydrogel has the potential to be used as a gel electrolyte of a zinc ion battery. In order to endow hydrogel with better mechanical properties such as elasticity and compressibility, the N' N-dimethyl bisacrylamide is adopted to chemically crosslink monomer acrylamide, and ammonium persulfate is used for initiating polymerization of monomers, compared with a preparation method in the prior art that polyacrylamide is directly mixed with other additives, the performance of the hydrogel has the advantages of difficult leakage, long storage time, difficult large-area oxidation crystallization, reduction of battery sealing requirements and the like, the preparation method and the used materials are simpler, the mechanical properties of electrolyte are greatly improved after crosslinking, and the hydrogel can achieve good compressibility similar to that of rubber materials (for example, good ionic conductivity can be maintained under 80% of compression strain). Meanwhile, the rechargeable zinc ion battery assembled by the crosslinked polyacrylamide also obtains good mechanical compressibility and electrochemical energy storage performance. Under the action of various compressive strains, the battery can show good electrochemical performances, such as specific charge-discharge capacity and cycle performance, and even reach or exceed the performances measured in aqueous solution.
(2) The rechargeable zinc-ion battery of the invention shows good electrochemical performance. Through detection, under the multiplying power of 1C, the discharge specific capacity of the battery reaches 230.5mAh g -1 The discharge specific capacity is 277.5mAh g measured under the same multiplying power in the similar aqueous solution -1 . Moreover, under the multiplying power of 1-5C, the battery shows good multiplying power conservation rate, and can still keep close to 140mAh g under the multiplying power of 5C -1 Specific discharge capacity of (a); at 4C rate, the initial capacity of the battery can be kept close to 70% after the battery is charged and discharged for 1000 circles.
(3) The rechargeable zinc-ion battery of the invention exhibits good compressibility and electrochemical performance. Through detection, under the condition of 25% pressure strain and 30-circle test, the cycle performance of the battery is kept stable and is not attenuated; even under the reciprocating strain of 0 to 20 percent, the specific capacity of the battery is almost not attenuated, but slightly increased; when the compressive strain is increased from 40 percent to 80 percent and then reduced to 40 percent, the specific capacity of the battery is kept stable and has no obvious change. Meanwhile, the output voltage of the battery is monitored, and the output voltage of the battery is kept stable and does not drop obviously even under external interference such as hand pressing and quick hammering.
(4) When the cell of the present invention is used to power a flexible pressure sensor, the stability of the output signal of the pressure sensor is similar to that of a commercial alkaline cell, and the cell of the present invention can maintain a stable output even under a compressed state. Moreover, its excellent compressibility and flexibility enable integration of the battery with the pressure sensor, reflecting its potential as a wearable smart device.
Drawings
FIG. 1 shows a structure of a battery and a method for synthesizing hydrogel by crosslinking.
FIG. 2 is a representation of hydrogel compressibility and ionic conductivity; wherein fig. 2 (a) is a photograph of compression and release of polyacrylamide gel, fig. 2 (b) is a photograph of a scanning electron microscope of freeze-dried polyacrylamide gel with a scale bar of 20 μm, fig. 2 (c) is a stress-strain curve of polyacrylamide gel at 5 consecutive cycles, fig. 2 (d) is an electrochemical impedance spectroscopy analysis of polyacrylamide gel at a compressive strain of from 0 to 77.8%, and fig. 2 (e) is a curve of change in resistance of polyacrylamide gel at a strain of from 0 to 77.8%; fig. 2 (f) and 2 (g) are photographs of polyacrylamide hydrogel in a normal state and a compressed state for conducting an electric circuit to light an LED lamp.
FIG. 3 is a representation of the electrochemical performance of a cell; wherein, fig. 3 (a) is the cyclic voltammetry curve of the rechargeable zinc-manganese battery in the polyacrylamide hydrogel, sweep rate: 5 millivolts/second; FIG. 3 (b) is the first two-turn charge-discharge curve of the battery at 1C rate; FIG. 3 (C) is a charge-discharge curve of the battery at 1-5C rate; FIG. 3 (d) is a performance curve of a battery charged and discharged 1000 cycles at 4C rate in a polyacrylamide hydrogel.
FIG. 4 is a cell compressibility and electrochemical stability characterization; wherein fig. 4 (a) is the cycling performance of the cell at 1C rate at 25% compressive strain; FIG. 4 (b) is the charge and discharge curves of 1,15 and 30 circles under 25% compressive strain of the cell; fig. 4 (C) is a charge-discharge curve for a cell at 0 and 20% strain and 1C rate for 7 cycles; fig. 4 (d) is the specific capacity of the battery at 0 and 20% cyclic pressure strain; fig. 4 (e) is a charge-discharge curve of a battery under a compressive strain from 40 to 80% and back to 40%; fig. 4 (f) is a specific capacity curve of a battery under a compressive strain from 40 to 80% and back to 40%; FIG. 4 (g) is the voltage stability of the battery under finger pressure; fig. 4 (h) shows the stability of the cell voltage under continuous hammering.
FIG. 5 is an illustration of the use of compressible batteries to power a pressure sensor and the integration of a battery sensor device; FIGS. 5 (a) -5 (c) are photographs of compressible batteries used to power the light panel; FIG. 5 (d) is a comparison of the performance of a compressible cell versus a commercial alkaline cell for powering a sensor; fig. 5 (e) is an integrated flexible smart bracelet based on a zinc ion battery and a flexible pressure sensor; FIG. 5 (f) is the sensor signals at different finger pressure levels; FIG. 5 (g) shows sensor signals at different frequencies from 0.3 to 4 Hz.
Detailed Description
The present invention will be further described with reference to the following description and examples, which include but are not limited to the following examples.
The embodiment provides a compressible rechargeable zinc-manganese battery, which consists of a positive electrode, a negative electrode and an electrolyte containing anions and cations and having ionic conductivity, wherein the negative electrode adopts an active material mainly containing zinc element, and the positive electrode active material is manganese dioxide. See fig. 1 and 2.
Specifically, the main purpose of this example is to improve the mechanical properties of the polymer electrolyte itself and the battery using this electrolyte, so this example develops and uses a chemically crosslinked polyacrylamide hydrogel as the electrolyte of the rechargeable zinc ion battery, compared with the common battery separator, the polyacrylamide hydrogel has good water retention property and is compatible with the ions in the zinc ion electrolyte, and in order to give better mechanical properties to the hydrogel, such as elasticity and compressibility, the present invention uses N' N-dimethyl bisacrylamide to chemically crosslink monomer acrylamide, and at the same time uses ammonium persulfate to initiate polymerization monomer. The specific synthesis method comprises the following steps: adding 3-5 g of monomer acrylamide, 25-35 mg of ammonium persulfate initiator and 3-5 mg of N' N-dimethyl bisacrylamide into 15-25 ml of deionized water, and continuously stirring until the mixture is clear; then transferring the clear solution into a glass surface vessel, coating the glass surface vessel with tinfoil paper, and reacting at 50-70 ℃ for 50-70 min to obtain hydrogel; finally, the hydrogel is placed in 0.8-1.2 mol/L zinc sulfate and 0.05-0.15 mol/L manganese sulfate electrolyte for full soaking, and the cross-linked polyacrylamide hydrogel electrolyte is obtained. The polyacrylamide hydrogel obtains good elasticity thanks to chemical crosslinking, and in particular, in addition to obtaining better compressibility, the electrochemical properties of the cell itself can be well maintained or even improved, thanks to the adequate contact of the electrolyte with the electrode material and to the improved ionic conductivity. The open circuit voltage of the battery shows good stability under external disturbances such as pressing and hammering. Due to the electrolyte, the preparation of integrated devices such as flexible sensors and batteries can be realized, and the electrolyte has wide prospect for application on wearable equipment in the future.
In the embodiment, the negative electrode material of the rechargeable zinc ion battery is prepared by an electrodeposition method. Specifically, the negative electrode material is prepared by electrodeposition of graphite paper serving as a current collector under a three-electrode system by a potentiostatic method of-1.3 to-1.5V, and an electrolyte used in the electrodeposition process contains 0.1 to 0.3mol/L of zinc sulfate and 0.4 to 0.6mol/L of sodium citrate. The positive active material manganese dioxide is prepared by a hydrothermal method, and the method specifically comprises the following steps: fully mixing 0.02-0.04 mol of manganese sulfate, 1-3 ml of 0.4-0.6 mol/L sulfuric acid, 80-100 ml of deionized water and 15-25ml of 0.0.05-0.15 mol/L potassium permanganate at room temperature to obtain a mixed solution; then transferring the mixed solution into water for hot compress and reacting for 10-14 h at 100-140 ℃; then washing the hydrothermal product with deionized water to be neutral and drying in vacuum to obtain dried manganese oxide; mixing the dried manganese oxide, acetylene black serving as a conductive agent and polyvinylidene fluoride serving as a binder in N' -methyl pyrrolidone according to the proportion of 7. And attaching the positive and negative electrode materials to the prepared polyacrylamide hydrogel electrolyte to assemble the battery.
Referring to FIGS. 3 and 4, assembled using the polyacrylamide hydrogel electrolyteThe rechargeable zinc-ion battery exhibits good electrochemical performance. Through detection, under the multiplying power of 1C, the discharge specific capacity of the battery reaches 230.5mAh g -1 The discharge specific capacity is 277.5mAh g measured under the same multiplying power in the similar aqueous solution -1 . Besides, under the multiplying power of 1-5C, the battery shows good multiplying power conservation rate, and can still keep close to 140mAhg at 5C -1 Specific discharge capacity of (2). At 4C rate, the initial capacity of the battery can be kept close to 70% after the battery is charged and discharged for 1000 circles.
A rechargeable zinc ion battery assembled by the polyacrylamide hydrogel electrolyte has good compressibility and electrochemical performance. Through detection, under the condition of 25% pressure strain and 30-circle test, the cycle performance of the battery is kept stable and does not attenuate. Even at a reciprocal strain of 0 to 20%, the specific capacity of the battery hardly decays, but rather rises slightly. When the compressive strain is increased from 40% to 80% and then decreased to 40%, the specific capacity of the battery is kept stable and has no obvious change. Meanwhile, the output voltage of the battery is monitored, and the output voltage of the battery is kept stable and does not drop obviously even under external interference such as hand pressing and quick hammering.
When used to power a flexible pressure sensor, the pressure sensor has a similar stability of the output signal compared to commercial alkaline batteries, and the battery of this embodiment maintains a stable output even under pressure. Furthermore, its excellent compressibility and flexibility allow successful integration of the battery with the pressure sensor, and therefore, referring to fig. 5, the present embodiment also provides a battery-sensor integrated device in which the battery is integrated with the pressure sensor.
The above-mentioned embodiment is only one of the preferred embodiments of the present invention, and should not be used to limit the scope of the present invention, but all the insubstantial modifications or changes made within the spirit and scope of the main design of the present invention, which still solve the technical problems consistent with the present invention, should be included in the scope of the present invention.
Claims (7)
1. A compressible rechargeable zinc-manganese battery is composed of a positive electrode, a negative electrode and an electrolyte containing anions and cations and having ionic conductivity, wherein the negative electrode adopts an active material mainly containing zinc element, the positive electrode active material is manganese dioxide, the electrolyte is a crosslinked polyacrylamide hydrogel electrolyte, and the synthesis method of the crosslinked polyacrylamide hydrogel electrolyte is as follows: adding 3-5 g of monomer acrylamide, 25-35 mg of ammonium persulfate initiator and 3-5 mg of N' N-dimethyl bisacrylamide into 15-25 ml of deionized water, and continuously stirring until the mixture is clear; then transferring the clear solution into a glass surface vessel, coating the glass surface vessel with tinfoil paper, and reacting at 50-70 ℃ for 50-70 min to obtain hydrogel; finally, the hydrogel is placed in 0.8-1.2 mol/L zinc sulfate and 0.05-0.15 mol/L manganese sulfate electrolyte for full soaking, and the cross-linked polyacrylamide hydrogel electrolyte is obtained.
2. The compressible rechargeable zinc-manganese dioxide battery as claimed in claim 1, characterized in that the negative electrode material is prepared by electrodeposition of graphite paper as a current collector under a three-electrode system under a potentiostatic method of-1.3 to-1.5V.
3. A compressible rechargeable zinc-manganese cell according to claim 2 wherein the electrolyte used in the electrodeposition process contains 0.1 to 0.3mol/L zinc sulphate and 0.4 to 0.6mol/L sodium citrate.
4. A compressible rechargeable zn-mn cell according to any one of claims 1 to 3, wherein the positive active material, manganese dioxide, is prepared by a hydrothermal process.
5. A compressible rechargeable zinc-manganese cell according to claim 4 wherein the hydrothermal preparation of manganese dioxide is as follows: fully mixing 0.02-0.04 mol of manganese sulfate, 1-3 ml of 0.4-0.6 mol/L sulfuric acid, 80-100 ml of deionized water and 15-25ml of 0.0.05-0.15 mol/L potassium permanganate at room temperature to obtain a mixed solution; then transferring the mixed solution into water for hot compress and reacting for 10-14 h at 100-140 ℃; then washing the hydrothermal product with deionized water to be neutral and drying in vacuum to obtain dried manganese oxide; mixing the dried manganese oxide, a conductive agent and a binder in N' -methyl pyrrolidone according to the proportion of 7.
6. A compressible rechargeable zinc manganese cell according to claim 5 wherein the conductive agent is acetylene black; the binder is polyvinylidene fluoride.
7. The battery-sensor integrated device according to claim 6, wherein the battery is integrated with a pressure sensor.
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Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111525185A (en) * | 2020-03-30 | 2020-08-11 | 东华大学 | Flexible zinc ion battery polymer electrolyte and preparation and application thereof |
| CN112103560A (en) * | 2020-09-16 | 2020-12-18 | 武汉大学 | Hygroscopic hydrogel-based battery and preparation method thereof |
| CN112310490A (en) * | 2019-07-31 | 2021-02-02 | 南京林业大学 | Preparation method of gel electrolyte for double-cross-linked-water-system metal ion energy storage device |
| CN112615086A (en) * | 2020-12-08 | 2021-04-06 | 中国科学院深圳先进技术研究院 | Flexible pressure sensor and polymer hydrogel electrolyte |
| CN112646074A (en) * | 2020-12-31 | 2021-04-13 | 江苏劲源新能源科技有限公司 | High-voltage self-repairing flexible hydrogel, preparation method thereof and battery containing hydrogel |
| CN112713010A (en) * | 2020-12-21 | 2021-04-27 | 浙江理工大学 | Method for preparing flexible planar micro energy storage device by laser printing sacrificial pattern and flexible planar micro energy storage device |
| CN112928342A (en) * | 2021-02-08 | 2021-06-08 | 安徽大学 | Multifunctional zinc ion micro battery and preparation method and application thereof |
| CN113078371A (en) * | 2021-03-25 | 2021-07-06 | 郑州大学 | Aqueous zinc ion battery electrolyte and preparation method and application thereof |
| CN113075276A (en) * | 2020-01-06 | 2021-07-06 | 青岛大学 | Preparation method of self-powered ionic hydrogel sensor, sensor and application |
| CN113285127A (en) * | 2020-02-19 | 2021-08-20 | 松山湖材料实验室 | Acid-base-resistant and compressible water-based zinc ion battery, electrolyte thereof and preparation method thereof |
| CN114122534A (en) * | 2020-08-28 | 2022-03-01 | 中国科学院上海硅酸盐研究所 | Zinc dendrite-resistant solid zinc-based battery electrolyte and preparation method thereof |
| CN114256516A (en) * | 2020-09-23 | 2022-03-29 | 天津大学 | Water-based zinc ion battery based on temperature response type self-protection electrolyte and preparation method and application thereof |
| CN114696037A (en) * | 2020-12-28 | 2022-07-01 | 陈璞 | Polymer gel electrolyte diaphragm, preparation method thereof and zinc ion battery |
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| CN112310490A (en) * | 2019-07-31 | 2021-02-02 | 南京林业大学 | Preparation method of gel electrolyte for double-cross-linked-water-system metal ion energy storage device |
| CN112310490B (en) * | 2019-07-31 | 2022-03-25 | 南京林业大学 | Preparation method of gel electrolyte for double-cross-linked-water-system metal ion energy storage device |
| CN113075276B (en) * | 2020-01-06 | 2023-10-27 | 青岛大学 | Preparation method of self-powered ionic hydrogel sensor, sensor and application |
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| CN112103560A (en) * | 2020-09-16 | 2020-12-18 | 武汉大学 | Hygroscopic hydrogel-based battery and preparation method thereof |
| CN112103560B (en) * | 2020-09-16 | 2021-11-26 | 武汉大学 | Hygroscopic hydrogel-based battery and preparation method thereof |
| CN114256516B (en) * | 2020-09-23 | 2023-11-21 | 天津大学 | Water-based zinc ion battery based on temperature response type self-protection electrolyte, and preparation method and application thereof |
| CN114256516A (en) * | 2020-09-23 | 2022-03-29 | 天津大学 | Water-based zinc ion battery based on temperature response type self-protection electrolyte and preparation method and application thereof |
| CN112615086A (en) * | 2020-12-08 | 2021-04-06 | 中国科学院深圳先进技术研究院 | Flexible pressure sensor and polymer hydrogel electrolyte |
| CN112713010A (en) * | 2020-12-21 | 2021-04-27 | 浙江理工大学 | Method for preparing flexible planar micro energy storage device by laser printing sacrificial pattern and flexible planar micro energy storage device |
| CN114696037A (en) * | 2020-12-28 | 2022-07-01 | 陈璞 | Polymer gel electrolyte diaphragm, preparation method thereof and zinc ion battery |
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| NL2030752A (en) * | 2021-02-08 | 2022-09-08 | Univ Anhui | Multi-functional zinc ion micro-battery and preparation method and application thereof |
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| CN113078371A (en) * | 2021-03-25 | 2021-07-06 | 郑州大学 | Aqueous zinc ion battery electrolyte and preparation method and application thereof |
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Application publication date: 20190426 |