CN112332021A - Method for avoiding thermal runaway of lithium ion battery - Google Patents
Method for avoiding thermal runaway of lithium ion battery Download PDFInfo
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- CN112332021A CN112332021A CN202011209398.1A CN202011209398A CN112332021A CN 112332021 A CN112332021 A CN 112332021A CN 202011209398 A CN202011209398 A CN 202011209398A CN 112332021 A CN112332021 A CN 112332021A
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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
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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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
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
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- Y02E60/10—Energy storage using batteries
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Abstract
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a method for avoiding thermal runaway of a lithium ion battery; the method comprises the following steps: (1) surface activation of raw vermiculite powder: grinding raw vermiculite into powder, cleaning the raw vermiculite powder, dynamically soaking the raw vermiculite powder in an acidic solution or an alkaline solution, and then drying the raw vermiculite powder after solid-liquid separation; (2) preparing a dispersion liquid: fully mixing and dissolving a solvent, a surfactant, a dispersant and a binder, adding raw vermiculite powder, stirring uniformly, and then adjusting the viscosity of the slurry to be 1000-20000mPa & S; (3) coating and baking; the method can improve the safety performance of the lithium ion battery and avoid the thermal runaway phenomenon.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a method for avoiding thermal runaway of a lithium ion battery.
Background
"thermal runaway" refers to an overheating phenomenon in which an exothermic chain reaction occurs inside a battery, causing a rapid change in the rate of temperature rise of the battery. When thermal runaway occurs in a lithium ion power battery, the most direct manifestation is a sharp rise in temperature accompanied by extreme conditions such as fire, explosion, and the like. Therefore, thermal runaway of the lithium ion battery due to short circuit is a major problem in battery safety design.
Patent application number CN201911359279.1 discloses a lithium ion battery of high security in order to prevent the thermal runaway that causes because the inside short circuit of battery, specifically is that battery case inner wall has expandable graphite coating, expandable graphite coating's principal ingredients includes expandable graphite and fire prevention auxiliary agent, because expandable graphite is heated the inflation back, the volume increases rapidly, wraps up electric core rapidly, so can completely cut off electric core and outside air contact, reach fire-retardant effect to realize the inside short circuit protection of electric core. On one hand, however, because the expandable graphite expands along with the change of temperature in a larger temperature range, and the expansion property of the expandable graphite does not have temperature selectivity, even in the temperature range (-20 ℃ -80 ℃) of the normal use of the battery, when the temperature of the battery changes, the expandable graphite still undergoes obvious volume expansion, so that the cell and the shell in the battery case can be stressed, the cell and the shell of the battery can be deformed, the performance of the battery can be affected, and even the safety problems such as internal short circuit of the battery can be caused by the deformation of the cell; on the other hand, because the potential safety hazards such as thermal runaway of the battery mainly start from the problems of overheating or short circuit inside the battery cell, and inflammable and explosive substances mainly exist inside the battery cell and are irrelevant to the battery shell and the interface between the battery shell and the battery cell, the potential safety hazards when the battery cell has problems can not be effectively solved by simply adding the expandable graphite coating on the inner wall of the battery shell.
Patent application No. CN201510968923.0 discloses a lithium ion battery with high security, can be at the battery because improper charging, the short circuit or expose in adverse circumstances such as high temperature and when unexpected, in time cut off the reaction of battery, prevent that the battery from producing thermal runaway, can guarantee the security performance of battery, guarantee lithium ion battery's normal use, specifically coat respectively at the top surface and the bottom surface of anodal mass flow body and scribble the anodal thermal expansion material layer of one deck, coat respectively at the top surface and the bottom surface of negative pole mass flow body and scribble one deck negative pole thermal expansion material layer. However, the method has the following defects: but (1) the expandable material layer has low conductivity, so that the electron transmission between the material and the current collector is influenced, the internal resistance of the battery is increased, and the performance of the battery is reduced; (2) the expandable material layer expands along with the change of temperature in a larger temperature range, and the expansion property of the expandable material layer has no temperature selectivity, so that even in the temperature range of normal use of the battery (minus 20-80 ℃), when the temperature of the battery changes, the expandable material layer still undergoes obvious volume expansion, and a charge transmission path between a positive electrode material and a negative electrode material and a current collector is cut off, so that the battery cannot work normally; (3) because the expandable material layer is respectively coated on the top surface and the bottom surface of the positive and negative current collectors and is positioned between the positive and negative active materials and the current collectors, when the temperature of the battery is increased and decreased within the normal use temperature range, the volume of the expandable material layer can also be expanded and contracted, and the volumes of the positive and negative active material layers and the current collector layers positioned on the upper part and the lower part of the expandable material layer are basically unchanged, so that strong stress can be generated between the expandable material layer and the positive and negative active material layers as well as between the expandable material layer and the current collector layers, and further the expandable material layer, the positive and negative active material layers and the current collector layers are.
In addition, the expandable graphite has high production cost, which is not beneficial to mass production and industrial application; the vermiculite has the performance of thermal expansion and the temperature selectivity, the volume expansion ratio reaches 10-20 times, but most of the vermiculite in China is used for building heat insulation and fire prevention materials after being prepared into expanded vermiculite at present, so that the invention provides a new idea for solving the thermal runaway of the lithium ion battery based on the expansion performance of raw vermiculite.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a method for avoiding thermal runaway of a lithium ion battery.
The method is realized by the following technical scheme:
a method for avoiding thermal runaway of a lithium ion battery is characterized in that raw vermiculite powder subjected to surface activation is coated on the surface of any one or more of a positive plate, a negative plate and a diaphragm; the surface activation is to wash the raw vermiculite powder, dynamically soak the raw vermiculite powder for 1 to 20 hours by adopting an acid solution or an alkaline solution, the soaking temperature is less than or equal to 90 ℃, and then dry the raw vermiculite powder after solid-liquid separation.
The particle size of the raw vermiculite powder is 0.001-1 mu m.
The concentration of the acid solution is 0.01-5 mol/L.
The modified functional group of the acidic solution is at least hydrogen ions; specifically, the acid is any one of perchloric acid, hydroiodic acid, sulfuric acid, hydrobromic acid, hydrochloric acid, nitric acid, iodic acid, oxalic acid, sulfurous acid, phosphoric acid, pyruvic acid, nitrous acid, citric acid, hydrofluoric acid, malic acid, gluconic acid, formic acid, lactic acid, benzoic acid, acrylic acid, acetic acid, propionic acid, bisulfic acid, hypochloric acid, and boric acid.
The concentration of the alkaline solution is 0.01-5 mol/L.
The alkaline solution has a modification functional group of at least hydroxide ions; specifically, sodium hydroxide, potassium hydroxide, barium hydroxide, sodium carbonate, sodium bicarbonate, calcium hydroxide, ammonia water, calcium bicarbonate, methylamine, urea (urea), ethylamine, ethanolamine, ethylenediamine, dimethylamine, trimethylamine, triethylamine, propylamine, isopropylamine, 1, 3-propanediamine, 1, 2-propanediamine, tripropylamine, triethanolamine, butylamine, isobutylamine, tert-butylamine, hexylamine, octylamine, aniline, benzylamine, cyclohexylamine, pyridine, hexamethylenetetramine, 2-chlorophenol, 3-chlorophenol, 4-chlorophenol, o-aminophenol, m-aminophenol, p-aminophenol, o-toluidine, m-toluidine, p-toluidine, 8-hydroxyquinoline, diphenylamine, benzidine, n-butyllithium, potassium tert-butoxide, sodium tert-butoxide, pyridine, aromatic amine, sodium methoxide, potassium ethoxide, potassium tert-butoxide, butyllithium, phenyllithium, Lithium diisopropylamide and lithium hexamethyldisilazide.
Specifically, the method for avoiding the thermal runaway of the lithium ion battery comprises the following steps:
(1) surface activation of raw vermiculite powder: grinding raw vermiculite into powder, cleaning the raw vermiculite powder, dynamically soaking for 1-20h by adopting an acid solution or an alkaline solution at the soaking temperature of less than or equal to 90 ℃, and then drying after solid-liquid separation;
(2) preparing a dispersion liquid: fully mixing and dissolving a solvent, a surfactant, a dispersant and a binder, adding raw vermiculite powder, stirring uniformly, wherein the solid content of the raw vermiculite powder in the dispersion is 10-80%, and then adding the binder or the surfactant to adjust the viscosity of the slurry to be 1000-20000mPa S;
(3) coating: coating the dispersion on a pole piece or a diaphragm by adopting any one of transfer equipment, extrusion equipment, spray equipment, dipping and spraying, wherein the coating speed is 1-80m/min, the coating thickness is 5-500 mu m, and then baking.
The revolution speed of the dry mixing is 20-100 r/min, and the rotation speed is 500-.
The solvent is a common solvent in the production of the lithium ion battery; including but not limited to: n-methyl pyrrolidone, water, alcohols, esters and ethers.
The solvent is selected according to the type of the pole piece, and if the doping object is a positive pole piece, the non-aqueous solvent is selected; if the doping object is the negative plate, an aqueous solvent is selected.
The surfactant is any one of CMC, polyethylene glycol, sodium dodecyl benzene sulfonate, polyvinylpyrrolidone and hexadecyl trimethyl ammonium bromide.
The dispersing agent is any one of urea and polyvinylpyrrolidone.
The binder is any one of PVDF, styrene butadiene rubber, CMC, sodium alginate, polypropylene and polyurethane.
The raw vermiculite refers to unexpanded vermiculite, and has the advantages that: (1) when heated, the volume expansion multiple is high and reaches 10-20 times, and a small amount or thin layer of vermiculite can be coated to achieve the obvious effect of avoiding thermal runaway of the lithium ion battery; (2) the method has excellent temperature selectivity, the volume of raw vermiculite hardly changes along with the temperature change of the battery within the normal use temperature range of the battery, and the volume of the raw vermiculite can expand rapidly only at the initial stage of potential safety hazards such as thermal runaway and the like when the temperature of the battery exceeds the normal working temperature limit, and the temperature is higher than 150 ℃, so that the function is exerted; (3) the density is low, and the use of vermiculite does not cause the increase of the weight of the battery and the reduction of the energy density; (4) the raw materials are easy to obtain, the reserves are abundant, and the price is low. Meanwhile, when the battery is subjected to thermal runaway and the temperature is rapidly increased, raw vermiculite is rapidly expanded to be changed into expanded vermiculite, and the expanded vermiculite has the advantages that: (1) the battery has good electrical insulation, can prevent the conduction of electrons in the electrode, and can separate the short circuit between the inside and the outside of the battery, thereby preventing the battery from further heating and a series of safety problems caused by the heating. (2) Good heat resistance and thermal insulation, and thus can prevent the battery from being ignited and thus from exploding when safety problems occur.
According to the invention, the surfactant and the dispersant are adopted to adjust the viscosity, so that the raw vermiculite powder can be effectively prevented from agglomerating, and the dispersion uniformity is improved.
The invention uses acid liquor or alkali liquor to soak raw vermiculite, on one hand, the invention can remove magnetic metal, magnetic metal oxide, oil stain, dust and other impurities on the surface of raw vermiculite, prevent the impurities from affecting the performance of the battery, on the other hand, the invention can carry out functional group modification on the surface of raw vermiculite, so that the raw vermiculite has better compatibility with the electrolyte and the absorption of the raw vermiculite to the electrolyte is improved, the infiltration rate of the electrolyte can be improved, the uniform distribution of the electrolyte in the battery cell is facilitated, meanwhile, the vermiculite powder expanded by heating can rapidly absorb the electrolyte in the process of rapid temperature rise caused by potential safety hazard of the battery, so as to block lithium ion exchange between the anode and the cathode and internal short circuit of the battery, wherein, the inorganic acid and alkali is mainly modified by hydroxide radical and hydrogen ion, and the organic acid and alkali can be modified by corresponding organic groups of each organic acid and alkali except the hydroxide radical and the hydrogen ion.
According to the invention, raw vermiculite powder is coated on the surfaces of the positive and negative pole pieces or the diaphragm, the action position is on the surfaces of the positive pole piece, the negative pole piece or the diaphragm, and when the temperature of the battery rapidly rises to generate potential safety hazards, the raw vermiculite on the surfaces of the positive pole piece, the negative pole piece or the diaphragm rapidly expands, so that on one hand, the distance between the positive pole and the negative pole is rapidly increased, and the expanded vermiculite is positioned between the positive pole and the negative pole to isolate the positive pole and the negative pole, so that the internal short circuit of the battery caused by the contact of; on the other hand, a large number of pores are generated in the expanded raw vermiculite, so that the battery electrolyte is adsorbed, the transmission of lithium ions between the anode and the cathode is blocked, and the internal reaction of the battery is cut off. Therefore, under the action of the two aspects, when the temperature of the battery sharply rises, the raw vermiculite coated on the surfaces of the positive plate, the negative plate or the diaphragm can effectively prevent the internal short circuit of the battery and prevent the electrochemical reaction from continuing, so that the thermal runaway of the lithium ion battery is avoided, and the safety and the electrochemical performance of the battery can be ensured.
Has the advantages that:
1. the method can improve the safety performance of the lithium ion battery and avoid the thermal runaway phenomenon;
the raw vermiculite powder is coated on the pole piece or the diaphragm, and the raw vermiculite powder subjected to surface activation treatment can expand by 10-20 times and generate a large number of pores when being heated to more than 150 ℃, so that the space between the positive plate and the negative plate can be enlarged, the electrolyte can be adsorbed, the positive plate and the negative plate can be isolated, a charge path and an internal short circuit between the positive plate and the negative plate in the battery can be cut off, the safety problem of the battery can be prevented, and the danger of thermal runaway of the battery can be effectively avoided. In addition, as the vermiculite before thermal expansion is small in volume and light in weight, the coating amount is effectively controlled, and the adverse effect on the energy density of the lithium ion battery can be avoided.
2. The method can effectively isolate the direct contact between the electrode and the electrolyte; the electrode material is protected from the corrosion of the electrolyte and the side reaction of the electrode/electrolyte interface is inhibited, thereby improving the cycling stability and the service life of the battery.
3. The method is simple, convenient for industrial application, cheap in raw materials, rich in reserves and low in cost, and the used solvent, surfactant, dispersant and binder are common reagents in the field, can be sold in the market and do not need to be specially prepared.
4. The method solves the unsafe problems caused by rapid temperature rise and thermal runaway of the lithium ion battery due to overcharge, heating, collision, penetration of a diaphragm by lithium dendrite, short circuit and the like, and tests show that the method can also avoid the thermal runaway and explosion of the battery even under the extreme conditions of needling extrusion and the like.
Drawings
FIG. 1: the charge and discharge curves of the lithium ion battery in example 4;
FIG. 2: electron micrographs of raw vermiculite;
FIG. 3: electron micrographs of exfoliated vermiculite;
FIG. 4: a photograph of the lithium ion battery in example 4 after the short circuit test;
FIG. 5: example 4 is a schematic diagram of the mechanism of action of raw vermiculite in lithium ion batteries.
Detailed Description
The following is a detailed description of the embodiments of the present invention, but the present invention is not limited to these embodiments, and any modifications or substitutions in the basic spirit of the embodiments are included in the scope of the present invention as claimed in the claims.
Example 1
A method for avoiding thermal runaway of a lithium ion battery comprises the following steps:
(1) surface activation of raw vermiculite powder: grinding raw vermiculite into powder with the particle size of 0.001 mu m, cleaning the raw vermiculite powder, dynamically soaking the raw vermiculite powder in a 2-chlorophenol solution with the concentration of 5mol/L for 1 hour, wherein the soaking temperature is less than or equal to 90 ℃, and then drying the raw vermiculite powder after solid-liquid separation;
(2) preparing a dispersion liquid: fully mixing and dissolving a non-aqueous solvent, a surfactant cetyl trimethyl ammonium bromide, a dispersant urea and a binder polyvinylidene fluoride, adding raw vermiculite powder, stirring uniformly, wherein the solid content of the raw vermiculite powder in the dispersion liquid is 10%, and then adding the binder or the surfactant to adjust the viscosity of the slurry to 20000mPa & S;
(3) coating: the dispersion liquid is coated on a positive plate by adopting a spray type device, the coating speed is 1m/min, the coating thickness is 500 mu m, and then the positive plate is baked.
Example 2
A method for avoiding thermal runaway of a lithium ion battery comprises the following steps:
(1) surface activation of raw vermiculite powder: grinding raw vermiculite into powder with the particle size of 1 mu m, cleaning the raw vermiculite powder, dynamically soaking the raw vermiculite powder for 20 hours by adopting a lactic acid solution with the concentration of 0.01mol/L, wherein the soaking temperature is less than or equal to 90 ℃, and then drying the raw vermiculite powder after solid-liquid separation;
(2) preparing a dispersion liquid: fully mixing and dissolving an aqueous solvent, a surfactant sodium carboxymethyl cellulose, a dispersant polyvinylpyrrolidone and a binder styrene butadiene rubber, adding raw vermiculite powder, stirring uniformly, wherein the solid content of the raw vermiculite powder in a dispersion liquid is 80%, and then adding the binder or the surfactant to adjust the viscosity of the slurry to be 1000mPa & S;
(3) coating: the dispersion liquid is coated on a negative plate by adopting a spraying mode, the coating speed is 80m/min, the coating thickness is 5 mu m, and then the negative plate is baked.
Example 3
A method for avoiding thermal runaway of a lithium ion battery comprises the following steps:
(1) surface activation of raw vermiculite powder: grinding raw vermiculite into powder with the particle size of 0.001-1 mu m, cleaning the raw vermiculite powder, dynamically soaking the raw vermiculite powder for 5 hours by using a urea solution with the concentration of 0.1mol/L, then dynamically soaking the raw vermiculite powder for 8 hours by using a phosphoric acid solution with the concentration of 3.8mol/L, wherein the soaking temperature is less than or equal to 90 ℃, and then drying the raw vermiculite powder after solid-liquid separation;
(2) preparing a dispersion liquid: fully mixing and dissolving a non-aqueous solvent, a surfactant sodium carboxymethyl cellulose, a dispersant polyvinylpyrrolidone and a binder polyvinylidene fluoride, adding the raw vermiculite powder, stirring uniformly, wherein the solid content of the raw vermiculite powder in the dispersion liquid is 45%, and then adding the binder or the surfactant to adjust the viscosity of the slurry to 13000mPa & S;
(3) coating: the HNT/PVDF composite separator was immersed in the dispersion, coated to a thickness of 80 μm, and then baked.
Example 4
The positive plate and the negative plate obtained in example 1 and example 2, and the HNT/PVDF composite separator were assembled into a lithium ion battery, and a charge and discharge test was performed under the conditions of 3.0 to 4.2V and 0.1C, and the results are shown in fig. 1, from which it can be seen that: the lithium ion battery has better charging and discharging capacity.
Claims (10)
1. A method for avoiding thermal runaway of a lithium ion battery is characterized in that surface activated vermiculite powder is coated on the surface of any one or more of a positive plate, a negative plate and a diaphragm; the surface activation is to wash the raw vermiculite powder, dynamically soak the raw vermiculite powder for 1 to 20 hours by adopting an acid solution or an alkaline solution, the soaking temperature is less than or equal to 90 ℃, and then dry the raw vermiculite powder after solid-liquid separation.
2. The method for preventing thermal runaway of a lithium ion battery according to claim 1, wherein the vermiculite powder has a particle size of 0.001 to 1 μm.
3. The method for avoiding thermal runaway of a lithium ion battery according to claim 1, wherein the concentration of the acidic solution is 0.01mol/L to 5 mol/L.
4. The method for avoiding thermal runaway of a lithium ion battery according to claim 1, wherein the concentration of the alkaline solution is 0.01mol/L to 5 mol/L.
5. The method for avoiding thermal runaway of a lithium ion battery according to any one of claims 1 to 4, comprising the following steps:
(1) surface activation of raw vermiculite powder: grinding raw vermiculite into powder, cleaning the raw vermiculite powder, dynamically soaking for 1-20h by adopting an acid solution or an alkaline solution at the soaking temperature of less than or equal to 90 ℃, and then drying after solid-liquid separation;
(2) preparing a dispersion liquid: fully mixing and dissolving a solvent, a surfactant, a dispersant and a binder, adding raw vermiculite powder, stirring uniformly, wherein the solid content of the raw vermiculite powder in a dispersion liquid is 10-80%, and then adding the binder or the surfactant to adjust the viscosity of the slurry to be 1000-20000mPa S;
(3) coating: coating the dispersion on a pole piece or a diaphragm by adopting any one of transfer equipment, extrusion equipment, spray equipment, dipping and spraying, wherein the coating speed is 1-80m/min, the coating thickness is 5-500 mu m, and then baking.
6. The method as claimed in claim 5, wherein the dry mixing has a revolution speed of 20-100 rpm and a rotation speed of 500-5000 rpm.
7. The method for avoiding thermal runaway of a lithium ion battery according to claim 5, wherein the solvents include but are not limited to: n-methyl pyrrolidone, water, alcohols, esters and ethers.
8. The method for avoiding thermal runaway of a lithium ion battery according to claim 5, wherein the surfactant is any one of CMC, polyethylene glycol, sodium dodecylbenzene sulfonate, polyvinylpyrrolidone and cetyltrimethylammonium bromide.
9. The method for avoiding thermal runaway of a lithium ion battery according to claim 5, wherein the dispersant is any one of urea and polyvinylpyrrolidone.
10. The method for avoiding thermal runaway of a lithium ion battery according to claim 1, wherein the binder is any one of PVDF, styrene butadiene rubber, CMC, sodium alginate, polypropylene and polyurethane.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN113193298A (en) * | 2021-04-16 | 2021-07-30 | 贵州梅岭电源有限公司 | Preparation method and application of ultrathin carbon-coated diaphragm |
| CN115483504A (en) * | 2022-10-13 | 2022-12-16 | 吉林师范大学 | Vermiculite coating diaphragm for lithium ion battery and preparation method thereof |
| CN116581243A (en) * | 2023-07-12 | 2023-08-11 | 宁德时代新能源科技股份有限公司 | Electrode plate, preparation method thereof, secondary battery and power utilization device |
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