CN113707931A - High-rate rapid charging and discharging aluminum ion battery and preparation method thereof - Google Patents

High-rate rapid charging and discharging aluminum ion battery and preparation method thereof Download PDF

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Publication number
CN113707931A
CN113707931A CN202111008025.2A CN202111008025A CN113707931A CN 113707931 A CN113707931 A CN 113707931A CN 202111008025 A CN202111008025 A CN 202111008025A CN 113707931 A CN113707931 A CN 113707931A
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aluminum
nano
ion battery
coating
methyl
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Inventor
程方生
李宏科
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Huixiang Energy Technology Suzhou Co ltd
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Huixiang Energy Technology Suzhou Co ltd
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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
    • H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
    • 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
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • 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
    • H01M10/058—Construction or manufacture
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/431—Inorganic material
    • H01M50/434—Ceramics
    • 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
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

The invention discloses a high-rate rapid charging and discharging aluminum ion battery and a preparation method thereof. The aluminum ion battery comprises a positive plate, a negative plate, a ceramic diaphragm, electrolyte and a battery case, wherein the positive plate, the ceramic diaphragm, the negative plate and the ceramic diaphragm are sequentially and repeatedly laminated to form a dry battery core, and the aluminum ion battery is prepared by putting the dry battery core into the battery case, injecting the electrolyte, opening the dry battery core to form the dry battery core, sealing the dry battery core and dividing the dry battery core into the battery case. By optimizing the application of the optimized material and the process technology, the prepared aluminum ion battery can be rapidly charged at the rate of 6C and discharged at the rate of 1C, and the charge-discharge capacity retention rate is up to more than 90%.

Description

High-rate rapid charging and discharging aluminum ion battery and preparation method thereof
Technical Field
The invention belongs to the technical field of secondary ion battery processes, and relates to a high-rate rapid charging and discharging aluminum ion battery and a preparation method thereof.
Background
With the vigorous development of new energy industry, secondary ion batteries have been widely used in various fields because of their advantages of high energy density, high power density, long cycle life, no memory effect, low self-discharge rate, wide working temperature range, safety, reliability, environmental friendliness, etc.
At present, the process technology of commercial secondary ion batteries is relatively mature, the performances of rapid charge and discharge and the like are obviously optimized and improved, but the breakthrough is difficult to be made on the aspect of high-rate rapid charge and discharge performance, and particularly the high capacity retention rate is difficult to be realized on the aspect of rate discharge performance of more than 10C.
Under the background, the invention provides the high-rate rapid charging and discharging aluminum ion battery and the preparation method thereof to make up the defects of the prior art, thereby solving the problem of high-rate rapid discharging of the secondary ion battery.
Disclosure of Invention
The invention provides a high-rate rapid charging and discharging aluminum ion battery and a preparation method thereof, which improve the ion storage space, the specific surface area, the pore volume and the number of pores of an active material of a positive plate, and increase the migration and transmission channels of ions, thereby enhancing the rapid and stable embedding/de-embedding of the ions, solving the problem of rapid high-rate charging and discharging of the battery, and simultaneously improving the energy density of the battery; the capacity retention rate of 10C/1C charge and discharge relative to 1C/1C charge and discharge reaches more than 90 percent.
The technical scheme adopted by the invention is as follows:
a high-rate rapid charge-discharge aluminum ion battery comprises a dry battery core, wherein the dry battery core comprises a positive plate, a negative plate and a ceramic diaphragm, and all parts are sequentially and repeatedly laminated to form the high-rate rapid charge-discharge aluminum ion battery; the aluminum ion battery is prepared by putting a dry battery core into a battery shell, injecting electrolyte, forming, sealing and grading.
The positive plate is prepared by uniformly coating dried positive material, conductive agent and binder into slurry on the front and back surfaces of the nano microporous superconducting carbon-coated titanium mesh with the reserved tabs to form a positive plate coating, and drying and rolling the positive plate to obtain the positive plate with the thickness of 0.1-0.5 mm.
The negative plate is a nano microporous aluminum foil and is obtained by rolling the aluminum foil with the reserved tab through nano needling, the thickness of the negative plate is 0.6-1 mm, and the aperture of the nano micropore is 30-100 nm.
The positive and negative both sides coating nanometer alumina coating of diaphragm to with the help of the vacuum baking oven solvent in removing the alumina coating obtains, and ceramic diaphragm thickness is 6 ~ 30um, and ceramic diaphragm's area is greater than the area of positive/negative pole piece.
The electrolyte is prepared by combining and mixing aluminum halide salt, imidazolium salt, alkyl halide, carbonate and/or carboxylic ester organic solvent; the aluminum halide salt is aluminum chloride and aluminum bromide; the imidazole salt is 1-methyl-3-ethyl imidazole chloride, 1-ethyl-3-methyl imidazole chloride, 1-methyl-3-ethyl imidazole bromide and 1-ethyl-3-methyl imidazole bromide; the alkyl halide is M-halogenated N alkyl, M is 1, 2, 3, 4, 5, …, N is methyl, ethyl, propyl, butyl, pentyl, …, and the halogen is chlorine or bromine; the carbonate is dimethyl carbonate, ethyl methyl carbonate and diethyl carbonate; the carboxylic ester is methyl formate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, methyl butyrate and ethyl butyrate.
The preparation method of the electrolyte comprises the following steps:
firstly, raw material treatment: baking and drying aluminum chloride and 1-ethyl-3-methylimidazole chloride respectively, and removing water; respectively passing tetrachloromethane, diethyl carbonate and methyl formate through a core filter, an adsorption column, a purification column and a molecular sieve to remove impurities and water;
mixing and dispersing: putting aluminum chloride and 1-ethyl-3-methylimidazole chloride into a tetrachloromethane solvent, mixing and stirring, and fully and uniformly dispersing to obtain an anhydrous aluminum chloride ion solution; the molar ratio of the aluminum ions to the chloride ions is 1: 3.5-4;
physical modification: mixing and stirring the anhydrous aluminum chloride ion solution, diethyl carbonate and methyl formate, and fully and uniformly dispersing to obtain the anhydrous aluminum chloride ion electrolyte with low viscosity and high fluidity; the concentration of aluminum chloride ions is 4-16 mol/L;
the active material of the positive plate is prepared by combining and mixing porous composite carbon, fullerene and graphene, wherein the mixing ratio is 30 percent to 60 percent to 10 percent; the porous composite carbon has a pore diameter of 20-50 nm and a specific surface area of 200-500 m2(ii)/g, pore volume greater than 95%; the specific surface area of the fullerene is 1000-1500 m2(ii)/g; the specific surface area of the graphene is 2000-3000 m2/g；
The positive electrode conductive agent is one or the combination of more than two of superconductive carbon black, conductive graphite, carbon fiber and carbon nano tube.
The positive binder is one or the combination of more than two of polyvinylidene fluoride, styrene butadiene rubber and sodium carboxymethyl cellulose.
The nanometer micropore superconducting carbon-coated titanium mesh is obtained by coating a nanometer super conductive carbon coating on the surface of a high-porosity titanium mesh, not coating the titanium mesh on which a lug is reserved, and removing a solvent in the super conductive carbon coating by using a vacuum baking oven, wherein the thickness of the nanometer micropore superconducting carbon-coated titanium mesh is 6-20 mu m, and the pore diameter of the nanometer micropore is 30-100 nm.
The battery shell is square and is made of an aluminum-plastic film.
The high-rate rapid charging and discharging aluminum ion battery is safe and stable. The increase of the pore volume and the number of pores of the active material of the positive plate reduces the material volume drastic change effect caused by ion embedding and de-embedding in the charging and discharging process of the battery, improves the heat dissipation performance of the working process of the battery and further improves the safety and stability performance of the battery; the battery is completely matched without a heat dissipation cooling device in the using process, and fire, deflagration and explosion are basically avoided when the battery is impacted, extruded and needled by heavy objects.
In the application field of secondary ion batteries, in the market environment where lithium resources are in short supply and the price of lithium is high, the resources of aluminum and carbon are very rich, the processing is easier, and the cost advantage is very obvious, so that the raw material cost of the secondary ion battery is greatly reduced.
Detailed Description
The following describes specific embodiments of the present invention in detail with reference to the technical solutions.
A manufacturing method of a high-rate rapid charging and discharging aluminum ion battery comprises the following steps:
step 1, manufacturing a positive plate: preparing anode slurry from 85-98% by mass of an anode material, 1-10% by mass of a conductive agent and 1-15% by mass of a binder, uniformly coating the anode slurry on the front surface and the back surface of the nano microporous superconducting carbon-coated titanium mesh, and reserving a 5mm blank between the edges of the four directions of the anode coating plane and the edges of the nano microporous superconducting carbon-coated titanium mesh in the coating process; putting the anode plate into a vacuum baking oven, and baking the anode plate at 85 ℃ in a vacuum environment of-0.09 to-0.1 MPa to obtain an anode plate; rolling the positive plate to a compact state by using a calender, then putting the positive plate into a vacuum baking oven, and baking at 110 ℃ in a vacuum environment of-0.09 to-0.1 MPa to obtain the positive plate;
step 2, manufacturing the negative plate: rolling the aluminum foil with the thickness of 0.6-1 mm and reserved with the tabs by a nano-needle roller press, piercing the aluminum foil by a nano needle, and leaving a plurality of nano-micropores with the thickness of 30-100 nm on the aluminum foil to obtain a negative plate;
step 3, manufacturing the dry electric core: sequentially and repeatedly laminating the positive plate, the ceramic diaphragm, the negative plate and the ceramic diaphragm, wherein the reserved tab of the nano microporous superconducting carbon-coated titanium net of each positive plate is laminated and gathered, then wrapped by a metal sheet and welded to form a positive full tab, the reserved tab of the nano microporous aluminum foil of each negative plate is laminated and gathered, then wrapped by a metal sheet and welded to form a negative full tab, and the laminated outer surfaces in the positive/negative full tab direction and the reverse direction are wrapped by diaphragms to obtain a dry cell;
and step 4, assembling the battery: applying a certain pressure on a dry battery core at a certain temperature to enable the contact among the positive plate, the negative plate and the ceramic diaphragm to be more compact, then putting the dry battery core into a battery case, injecting electrolyte into the battery case, and obtaining the aluminum ion battery through formation, sealing and capacity grading.

Claims (8)

1. A high-rate rapid charge-discharge aluminum ion battery comprises a dry battery core, wherein the dry battery core comprises a positive plate, a ceramic diaphragm, a negative plate and a ceramic diaphragm, and all parts are sequentially and repeatedly laminated to form the high-rate rapid charge-discharge aluminum ion battery; the aluminum ion battery is prepared by putting a dry battery core into a battery shell, injecting electrolyte, opening, forming, sealing and grading; the method is characterized in that:
the positive plate is formed by uniformly coating dried positive material, conductive agent and binder into slurry on the front and back surfaces of the nano microporous superconducting carbon-coated titanium mesh with the reserved tabs to form a positive plate coating, and drying and rolling are carried out to obtain the positive plate with the integrated middle-surface density and middle-compacted density of the front and back materials, wherein the thickness of the positive plate is 0.1-0.5 mm;
the negative plate is a nano microporous aluminum foil and is prepared by rolling the aluminum foil with reserved lugs through nano needling, the thickness of the negative plate is 0.6-1 mm, and the aperture of the nano micropores is 30-100 nm;
coating the front surface and the back surface of the diaphragm with a nano aluminum oxide coating, and removing a solvent in the aluminum oxide coating by using a vacuum baking oven; the thickness of the ceramic diaphragm is 6-30 um, and the area of the ceramic diaphragm is larger than that of the positive/negative plate;
the electrolyte is prepared by combining and mixing aluminum halide salt, imidazolium salt, alkyl halide, carbonate and/or carboxylic ester organic solvent; the aluminum halide salt is aluminum chloride or aluminum bromide; the imidazole salt is one of 1-methyl-3-ethyl imidazole chloride, 1-ethyl-3-methyl imidazole chloride, 1-methyl-3-ethyl imidazole bromide and 1-ethyl-3-methyl imidazole bromide; the alkyl halide is M-halogenated N alkyl, wherein M is 1, 2, 3, 4, 5 and …, N is methyl, ethyl, propyl, butyl, pentyl and …, and halogen is chlorine or bromine; the carbonate is dimethyl carbonate, ethyl methyl carbonate and diethyl carbonate; the carboxylic ester is methyl formate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, methyl butyrate and ethyl butyrate.
2. The high-rate rapid charging and discharging aluminum ion battery as claimed in claim 1, wherein the active material of the positive plate is prepared by mixing porous composite carbon, fullerene and graphene, and the mixing ratio is 30% to 60% to 10%; the porous composite carbon has a pore diameter of 20-50 nm and a specific surface area of 200-500 m2(ii)/g, pore volume greater than 95%; the specific surface area of the fullerene is 1000-1500 m2(ii)/g; the specific surface area of the graphene is 2000-3000 m2/g。
3. The high-rate rapid charge-discharge aluminum ion battery according to claim 1 or 2, wherein the positive electrode conductive agent is one or a combination of two or more of superconducting carbon black, conductive graphite, carbon fiber and carbon nanotube.
4. The high-rate rapid charge-discharge aluminum ion battery according to claim 3, wherein the positive electrode binder is one or a combination of two or more of polyvinylidene fluoride, styrene butadiene rubber and sodium carboxymethylcellulose.
5. The high-rate rapid charging and discharging aluminum ion battery as claimed in claim 1, 2 or 4, wherein the nano-microporous superconducting carbon-titanium-coated mesh is obtained by coating a nano-super conductive carbon coating on the surface of a high-porosity titanium mesh, leaving no coating on the titanium mesh at the tab position, and removing the solvent in the super conductive carbon coating by means of a vacuum oven, wherein the thickness of the nano-microporous superconducting carbon-titanium-coated mesh is 6-20 μm, and the pore diameter of the nano-micropores is 30-100 nm.
6. The high-rate rapid charge-discharge aluminum ion battery according to claim 5, wherein the electrolyte is prepared by the following steps:
firstly, raw material treatment: baking and drying aluminum chloride and 1-ethyl-3-methylimidazole chloride respectively, and removing water; respectively passing tetrachloromethane, diethyl carbonate and methyl formate through a core filter, an adsorption column, a purification column and a molecular sieve to remove impurities and water;
mixing and dispersing: putting aluminum chloride and 1-ethyl-3-methylimidazole chloride into a tetrachloromethane solvent, mixing and stirring, and fully and uniformly dispersing to obtain an anhydrous aluminum chloride ion solution; the molar ratio of the aluminum ions to the chloride ions is 1: 3.5-4;
physical modification: mixing and stirring the anhydrous aluminum chloride ion solution, diethyl carbonate and methyl formate, and fully and uniformly dispersing to obtain the anhydrous aluminum chloride ion electrolyte with low viscosity and high fluidity; the concentration of aluminum chloride ions is 4-16 mol/L.
7. The battery can of claim 6, wherein the shape is square and the material is an aluminum plastic film.
8. The preparation method of the high-rate rapid charging and discharging aluminum ion battery as claimed in any one of claims 1 to 7, characterized by comprising the following steps:
A. manufacture of positive plate
Preparing anode slurry from 85-98% by mass of an anode material, 1-10% by mass of a conductive agent and 1-15% by mass of a binder, uniformly coating the anode slurry on the front surface and the back surface of the nano microporous superconducting carbon-coated titanium mesh, and reserving a 5mm blank between the edges of the four directions of the anode coating plane and the edges of the nano microporous superconducting carbon-coated titanium mesh in the coating process; putting the anode plate into a vacuum baking oven, and baking the anode plate at 85 ℃ in a vacuum environment of-0.09 to-0.1 MPa to obtain an anode plate; rolling the positive plate to a compact state by using a calender, then putting the positive plate into a vacuum baking oven, and baking at 110 ℃ in a vacuum environment of-0.09 to-0.1 MPa to obtain the positive plate;
B. manufacture of negative plate
Rolling the aluminum foil with the thickness of 0.6-1 mm and reserved with the tabs by a nano-needle roller press, piercing the aluminum foil by a nano needle, and leaving a plurality of nano-micropores with the thickness of 30-100 nm on the aluminum foil to obtain a negative plate;
C. dry cell fabrication
Sequentially and repeatedly laminating the positive plate, the ceramic diaphragm, the negative plate and the ceramic diaphragm, wherein the reserved tab of the nano microporous superconducting carbon-coated titanium net of each positive plate is laminated and gathered, then wrapped by a metal sheet and welded to form a positive full tab, the reserved tab of the nano microporous aluminum foil of each negative plate is laminated and gathered, then wrapped by a metal sheet and welded to form a negative full tab, and the laminated outer surfaces in the positive/negative full tab direction and the reverse direction are wrapped by diaphragms to obtain a dry cell;
D. battery assembly
And applying pressure to the dry cell to enable the contact among the positive plate, the negative plate and the ceramic diaphragm to be more compact, then putting the dry cell into a cell shell, injecting electrolyte into the cell shell, and performing opening formation, sealing and capacity grading to obtain the aluminum ion cell.
CN202111008025.2A 2021-08-31 2021-08-31 High-rate rapid charging and discharging aluminum ion battery and preparation method thereof Pending CN113707931A (en)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108376795A (en) * 2018-04-04 2018-08-07 天津大学 A kind of no dendrite, powerful aluminium ion battery
US20200287232A1 (en) * 2019-03-08 2020-09-10 Everon24, Inc. Aqueous aluminum ion batteries, hybrid battery-capacitors, compositions of said batteries and battery-capacitors, and associated methods of manufacture and use
CN112164828A (en) * 2020-09-22 2021-01-01 同济大学 Fibrous flexible aluminum ion battery and preparation method thereof

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108376795A (en) * 2018-04-04 2018-08-07 天津大学 A kind of no dendrite, powerful aluminium ion battery
US20200287232A1 (en) * 2019-03-08 2020-09-10 Everon24, Inc. Aqueous aluminum ion batteries, hybrid battery-capacitors, compositions of said batteries and battery-capacitors, and associated methods of manufacture and use
CN112164828A (en) * 2020-09-22 2021-01-01 同济大学 Fibrous flexible aluminum ion battery and preparation method thereof

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