CN111162322A - Preparation method of low-temperature lithium ion battery - Google Patents
Preparation method of low-temperature lithium ion battery Download PDFInfo
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- CN111162322A CN111162322A CN202010223479.0A CN202010223479A CN111162322A CN 111162322 A CN111162322 A CN 111162322A CN 202010223479 A CN202010223479 A CN 202010223479A CN 111162322 A CN111162322 A CN 111162322A
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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
- H01M10/058—Construction or manufacture
- H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
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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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- 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
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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
- 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
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Abstract
The invention relates to a preparation method of a low-temperature lithium ion battery, which comprises a porous positive plate with high electronic conductivity and high ionic conductivity, wherein an active material is a positive material of secondary micro-particles formed by primary nano-particles, a porous negative plate with high electronic conductivity and high ionic conductivity, an active negative material is a negative material of secondary micro-particles formed by primary nano-particles, a ceramic diaphragm with high porosity and high moistening property, and an electrolyte with low viscosity, low melting point and high low-temperature ionic conductivity. The lithium ion battery disclosed by the invention still keeps more than 80% of discharge capacity at an extremely low temperature (minus 45 ℃), has good low-temperature electrochemical performance, can expand the low-temperature working temperature range of the lithium ion battery, and solves the application of the lithium ion battery in electric vehicles and energy storage at extremely low temperature.
Description
Technical Field
The invention relates to the technical field of secondary batteries, in particular to a manufacturing method of a low-temperature lithium ion battery.
Background
The lithium ion battery has the advantages of high working voltage, high specific energy, long charging and discharging service life, low self-discharging rate, no memory effect and the like, so that the lithium ion battery has wider and wider application range in civil markets such as portable electronic equipment, electric tools and the like. But the poor low-temperature performance of the alloy material limits the application of the alloy material in special fields of aviation, aerospace, special communication, polar investigation, military and the like. For example, the low-temperature performance of the current lithium ion battery, especially the poor working performance in the low-temperature environment below-40 ℃, is mainly represented by the rapid attenuation of the discharge capacity and the reduction of the discharge voltage platform.
The main reasons influencing the low-temperature performance reduction of the lithium ion battery are that the transportation speed of lithium ions in the electrode and between the electrode and an electrolyte interface is reduced, and the migration and diffusion speed of electrons in the electrode and between the electrode and the electrolyte interface is reduced; secondly, the viscosity of the electrolyte increases at low temperature, and the ionic conductivity decreases. In addition, the porosity, pore size, specific surface area, electrode density, compaction, wettability of the electrode and the electrolyte at low temperature, and low temperature fluidity of the electrolyte of the lithium ion battery all affect the low temperature performance of the lithium ion battery.
The current methods for improving electron mobility generally adopt the addition of conductive agents (conductive carbon powder, carbon nanotubes, graphene, carbon nanowires, etc.) to the electrode active material. But only to a limited extent in improving the low temperature electrochemical performance in terms of improving electron transfer. The Chinese patent 201110055390.9 improves the low-temperature-20 ℃ electrochemical discharge capacity of the lithium-ion half cell by adding a lithium-ion conductor additive, namely perovskite type oxide, into the positive electrode. Chinese patent 201210134320.7 discloses that the stability of electrolyte can be maintained, the low-temperature conductivity can be improved, and the voltage plateau and discharge capacity of the battery can be improved at-20 ℃ by adjusting the porosity of positive and negative electrode plates and the composition of the electrolyte.
Disclosure of Invention
In order to solve the problems, the invention provides a manufacturing method of a low-temperature (less than minus 45 ℃) lithium ion battery.
The technical scheme of the invention is as follows:
a preparation method of a low-temperature lithium ion battery comprises a positive plate, a negative plate, a ceramic diaphragm and electrolyte, wherein the low temperature is less than minus 45 ℃; the preparation method comprises the following steps:
(1) positive plate
The active positive electrode material of secondary micron particles formed by primary nano particles and an electronic conductive additive are added with proper macromolecule plasticizer, and are coated on a carbon-coated aluminum foil through a binder, compacted and removed through a solvent extraction method to form a porous positive electrode plate.
(2) Negative plate
The active negative electrode material of secondary micron particles formed by primary nano particles and an electronic conductive additive are added with a proper macromolecular plasticizer, coated on a copper foil through a binder, compacted and removed through a solvent extraction method to form a porous negative electrode sheet.
(3) Electrolyte solution
A low viscosity, low melting point solvent is mixed with a lithium salt-solvent combination that still has a higher low temperature ionic conductivity at low temperatures to form an electrolyte.
(4) Ceramic diaphragm
The porous ceramic diaphragm with high porosity and high moistening performance at low temperature is selected.
(6) Assembled lithium battery
And (3) sequentially laminating the positive plate, the ceramic diaphragm and the negative plate prepared in the steps (1), (2) and (4), adding the electrolyte prepared in the step (3), and manufacturing according to a common soft package battery manufacturing process to finally obtain the low-temperature lithium ion battery.
The positive active material is one or a mixture of more of lithium cobaltate, lithium manganate, nickel cobalt manganese, lithium iron phosphate and nickel cobalt aluminum.
The negative active material is one or a mixture of more of lithium titanate, mesocarbon microbeads and artificial graphite (including hard carbon and soft carbon).
The surface density of the positive plate is 160-280 g/m 2; the compaction density is 1.0-2.8 g/cm 3; the surface density of the negative plate is 60-120 g/m 2; the compaction density is 0.8-1.6 g/cm 3; the positive electrode electronic conductive additive is KS6, carbon nano tube or VGCF or graphene or Super-P; the negative electrode electronic conductive additive is KS6, a carbon nano tube or VGCF or graphene or Super-P; the control of the compaction density and the surface density of the positive and negative electrode sheets and the selection of the electronic conductive additive are beneficial to the transmission of lithium ions at low temperature, and simultaneously, higher energy density is ensured.
The macromolecular plasticizer is DBP or PTP or DOP or DIDP; the low-viscosity and low-melting-point solvent is formed by mixing two solvents, wherein one solvent is carbonic ester, and the other solvent is ester; the carbonate is one or a mixture of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate and propyl methyl carbonate; the esters are one or a mixture of butyrolactone, methyl formate, ethyl formate, methyl acetate, ethyl propionate, methyl butyrate and ethyl butyrate.
The lithium salt is one or a mixture of more of LiPF6, LiBF4, LiBOB and LiBC2O4F 2; the concentration of the lithium salt is 0.7M-2M.
The binder is a mixture of at least one of polyvinylidene fluoride copolymer PVDF-HFP soluble in acetone, polyacrylonitrile, polyethylene terephthalate and polyethylene oxide.
The invention has the advantages of ingenious conception, reasonable design and the following beneficial effects,
(1) the positive plate formed by selecting an active positive electrode material and an electronic conductive additive, adding a proper macromolecule plasticizer and coating the active positive electrode material and the electronic conductive additive on the carbon-coated aluminum foil through a binder has the characteristics of high porosity, compact density and controllable surface density; the negative plate formed by selecting an active negative electrode material and an electronic conductive additive, adding a proper macromolecule plasticizer and coating the active negative electrode material and the electronic conductive additive on the carbon-coated copper foil through a binder has the characteristics of high porosity, compact density and controllable surface density; therefore, when lithium ions are transmitted at low temperature, the lithium ions are very smooth, and high energy density is ensured; meanwhile, by selecting a solvent with low viscosity and low melting point, a lithium salt-solvent combination with high low-temperature ionic conductivity at low temperature and a porous ceramic diaphragm with high porosity and high wettability at low temperature, the prepared lithium ion battery still keeps more than 80% of discharge capacity at extremely low temperature (-45 ℃) and has good low-temperature electrochemical performance. Therefore, the low-temperature working temperature range of the lithium ion battery is expanded, and the application of the lithium ion battery in electric vehicles and energy storage at extremely low temperature is solved.
(2) The macromolecular plasticizer is added in the preparation process of the positive and negative pole pieces, so that the energy density of the positive and negative pole pieces is not influenced in the forming process, the positive and negative pole pieces have high porosity, and the macromolecular plasticizer can be removed by a solvent extraction method in the subsequent process, so that the moistening property of the electrolyte at low temperature is ensured, the migration and diffusion speed of ions is improved, and the low-temperature electrochemical performance of the battery is improved.
(3) The solvent combination consisting of the solvent with low viscosity and low melting point and the lithium salt with higher low-temperature ionic conductivity at low temperature is adopted, so that the low-temperature ionic conductivity and the electron transmission rate are improved; the porous ceramic diaphragm with high porosity (more than 45 percent) is adopted to solve the wetting property and the migration and diffusion speed of ions at low temperature, improve the migration and transmission rate of lithium ions and electrons in the electrode and between the electrode and the electrolyte interface, improve the low-temperature ionic conductivity of the electrolyte, and solve the charging and discharging problems of the lithium ion battery under the application of extremely low temperature by combining multiple aspects.
The low-temperature performance of the lithium ion battery is comprehensively improved, the lithium ion battery has high energy density and high rate performance, and also has high low-temperature performance (-45 ℃ and the capacity can still be kept more than 80%), and the requirements of the battery products in the technical field of wider environmental temperature can be met.
Drawings
Fig. 1 is a schematic view of a lithium battery.
Fig. 2 is a schematic view of the internal structure of a lithium battery.
FIG. 3 is a schematic diagram of a discharge curve of a low-temperature lithium ion battery.
The positive plate 110 and the negative plate 120 of the lithium battery 100 are shown as a ceramic separator 130.
Detailed Description
As shown in fig. 1 and 2, a method for manufacturing a low-temperature lithium ion battery 100 includes the following steps,
step 1: 7 grams of polyvinylidene fluoride copolymer (PVDF-HFP) was added to 180 grams of acetone and dissolved by stirring thoroughly to form a viscous liquid.
Step 2: the manufacturing procedure of the positive electrode sheet 110 was performed as follows: 60 g of plasticizer DBP, 140g of lithium iron phosphate positive electrode material (lithium iron phosphate material with secondary micrometer particles formed by primary nanoparticles), 2.5% of carbon nanotube conductive agent and 1.5% of SP conductive agent are fully mixed and added into the viscous liquid, and the viscous positive electrode slurry is prepared by uniformly stirring the mixture by a stirrer. The obtained anode slurry is evenly coated on the carbon-coated aluminum foil on two sides, and the carbon-coated aluminum foil is kept in a vacuum oven at the temperature of 80 ℃ for 4 hours to remove the solvent acetone. The positive electrode sheet from which the solvent acetone was removed was densified using a calender, and the macromolecular plasticizer DBP in the positive electrode sheet was extracted with IPA and vacuum-dried at 110 ℃ to obtain a high porosity positive electrode sheet. The resulting positive electrode sheet had a compacted density of 1.8g/cm 3.
And step 3: the manufacturing procedure of the negative electrode sheet 120 is operated as follows: 7 g of polyvinylidene fluoride as a binder was added to 180 g of acetone and sufficiently stirred to be dissolved to form a viscous liquid. 60 g of plasticizer DBP, 70 g of composite carbon (secondary microparticle negative electrode material formed by primary nanoparticles), 1.5% of carbon nanotube conductive agent and 1.0% of SP conductive agent are fully mixed and added into the viscous liquid, and a stirrer is used for stirring uniformly to prepare viscous negative electrode slurry. And (3) uniformly coating the two surfaces of the obtained cathode slurry on copper foil, and keeping the cathode slurry in a vacuum oven at the temperature of 80 ℃ for 4 hours to remove the solvent acetone. The negative electrode sheet from which the solvent acetone was removed was densified using a calender, and the macromolecular plasticizer DBP in the negative electrode sheet was extracted by IPA and vacuum-dried at 110 ℃ to obtain a negative electrode sheet with high porosity. The obtained negative electrode sheet had a compacted density of 1.3g/cm 3.
And 4, step 4: the surface of the diaphragm is coated with a nano alumina coating by an electrostatic spinning method, and the solvent is removed in an oven to obtain the porous ceramic diaphragm 130 with high porosity and high wettability.
And 5: and adding a solvent with low viscosity and low melting point into the electrolyte solvent to obtain the lithium salt-solvent combination with high low-temperature ionic conductivity at low temperature.
Step 6: a preparation method of the lithium ion battery is provided: the positive electrode layer, the ceramic diaphragm layer and the negative electrode layer are sequentially stacked according to the sequence of the attached drawing 1, a certain pressure is applied at a certain temperature to enable the three layers to be in contact more compactly, electrolyte is added, the lithium ion battery 100 is manufactured according to the manufacturing process of a common soft package battery, and finally the low-temperature lithium ion battery 100 is obtained.
Fig. 3 shows a discharge curve of the lithium ion battery 100 at the low temperature. The retention rate of discharge capacity at high rate (10C) at minus 30 ℃ is more than 97 percent, and the retention rate of discharge capacity at 1C rate at minus 45 ℃ is more than 90 percent.
The above-mentioned embodiments only express one embodiment of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the present invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (9)
1. A preparation method of a low-temperature lithium ion battery comprises a positive plate, a negative plate, a ceramic diaphragm and electrolyte, wherein the low temperature is less than minus 45 ℃; the preparation method is characterized by comprising the following steps:
(1) positive plate
Adding a proper macromolecule plasticizer into an active positive electrode material and an electronic conductive additive which form secondary micron particles by primary nano particles, coating the active positive electrode material and the electronic conductive additive on a carbon-coated aluminum foil through a binder, and removing the active positive electrode material and the electronic conductive additive through a solvent extraction method to form a porous positive electrode plate;
(2) negative plate
Adding a proper macromolecule plasticizer into an active negative electrode material and an electronic conductive additive which form secondary micron particles by primary nano particles, coating the active negative electrode material and the electronic conductive additive on a copper foil through a binder, and removing the active negative electrode material and the electronic conductive additive through a solvent extraction method to form a porous negative electrode sheet;
(3) electrolyte solution
Mixing a low-viscosity and low-melting-point solvent and a lithium salt-solvent combination with high low-temperature ionic conductivity at low temperature to form an electrolyte;
(4) ceramic diaphragm
Selecting a porous ceramic diaphragm with high porosity and high moistening property at low temperature;
(5) lithium battery
Sequentially laminating the positive plate, the negative plate and the ceramic diaphragm prepared in the steps (1), (2) and (4), compacting, adding the electrolyte prepared in the step (3), and manufacturing according to a common manufacturing process of a soft package battery to finally obtain the low-temperature lithium ion battery.
2. The method for preparing the battery according to claim 1, wherein the positive active material is one or more of lithium cobaltate, lithium manganate, ternary nickel cobalt manganese, lithium iron phosphate and nickel cobalt aluminum.
3. The preparation method of the battery according to claim 1, wherein the negative active material is one or more of lithium titanate, mesocarbon microbeads and artificial graphite.
4. The method for preparing the battery according to claim 1, wherein the positive electrode sheet has an areal density of 120 to 280g/m 2; the compaction density is 1.0-2.8 g/cm 3; the surface density of the negative plate is 60-140 g/m2(ii) a The compaction density is 0.8-1.6 g/cm3。
5. The method for preparing the battery according to claim 1, wherein the positive electrode electron conductive additive is KS6, carbon nanotubes or VGCF or graphene Super-P; the negative electrode electronic conductive additive is KS6, carbon nano tube or VGCF or graphene or Super-P.
6. The method for manufacturing a battery according to claim 1, wherein the macromolecular plasticizer is DBP or PTP or DOP or DIDP.
7. The method of claim 1, wherein the low viscosity, low melting point solvent is formed by mixing two solvents, one of which is a carbonate and the other of which is an ester; the carbonate is one or a mixture of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate and propyl methyl carbonate; the esters are one or a mixture of butyrolactone, methyl formate, ethyl formate, methyl acetate, ethyl propionate, methyl butyrate and ethyl butyrate.
8. The method of claim 7, wherein the lithium salt-solvent combination is LiPF6、LiBF4、LiBOB、LiBC2O4F2A mixture of one or more of; the concentration of the lithium salt is 0.7M-2M.
9. The method for manufacturing a battery according to claim 1, wherein the binder is a mixture of at least one of polyvinylidene fluoride copolymer PVDF-HFP soluble in acetone, polyacrylonitrile, polyethylene terephthalate, and polyethylene oxide.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111952538A (en) * | 2020-06-18 | 2020-11-17 | 上海航天电源技术有限责任公司 | Preparation method of low-temperature battery and starting power supply based on low-temperature battery |
| CN112151853A (en) * | 2020-09-22 | 2020-12-29 | 浙江锋锂新能源科技有限公司 | Battery pole piece with melting recombination characteristic and lithium ion battery comprising same |
| CN112151755A (en) * | 2020-09-08 | 2020-12-29 | 江苏塔菲尔新能源科技股份有限公司 | Positive plate and battery |
| CN113086959A (en) * | 2021-02-26 | 2021-07-09 | 雅安锂盛新能企业管理中心(有限合伙) | High-compaction low-temperature lithium iron phosphate material, lithium battery positive plate and preparation method thereof |
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Application publication date: 20200515 |