CN110994030B - Lithium battery electrolyte and lithium ion battery - Google Patents
Lithium battery electrolyte and lithium ion battery Download PDFInfo
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- CN110994030B CN110994030B CN201911382877.0A CN201911382877A CN110994030B CN 110994030 B CN110994030 B CN 110994030B CN 201911382877 A CN201911382877 A CN 201911382877A CN 110994030 B CN110994030 B CN 110994030B
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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
- H01M10/056—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
- H01M10/0567—Liquid materials characterised by the additives
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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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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Abstract
The invention relates to the technical field of lithium ion battery materials, in particular to a lithium battery electrolyte and a lithium ion battery. The lithium battery electrolyte comprises an organic solvent, a lithium salt and an additive, wherein the additive comprises fluoroethylene carbonate and one or more than two of propane sulfonate pyridinium, dopamine, lithium difluoro oxalate borate and lithium difluoro phosphate. The electrolyte disclosed by the invention utilizes the synergistic effect of pyridinium propanesulfonate, dopamine, lithium difluoro-oxalato-borate and lithium difluoro-phosphate to replace the traditional propane sultone, so that the high-temperature storage and high-temperature cycle performance of the battery are improved, the low-temperature discharge capacity is greatly improved, and no harmful substances are generated; and simultaneously, the wettability of the electrolyte to an electrode material and a diaphragm is improved under a low-temperature condition by adopting ethyl acetate.
Description
Technical Field
The invention relates to the technical field of lithium ion battery materials, in particular to a lithium battery electrolyte and a lithium ion battery.
Background
The lithium ion battery is widely applied to the fields of portable electronic products and electric vehicles, and is expanded to the fields of electric automobiles, energy storage, military industry and the like. However, the application and popularization of the lithium ion battery also face the restrictions of specific energy and use environment, and the integration of the specific energy and the use environment to the lithium ion battery technology can be beneficial to becoming a technical short board at present.
Improving the specific capacity of the anode and cathode materials is an important means for improving the specific energy of the lithium ion battery. Wherein the application of high capacity silicon-based negative electrodes and high nickel ternary positive electrode materials is becoming increasingly common. However, the silicon-based negative electrode is accompanied by huge volume change in the lithium intercalation and deintercalation process, which can cause Si particle pulverization, electrode crack propagation, and unstable interface between the electrode and the electrolyte, and finally cause rapid capacity fading. The high-valence transition metal ions with strong oxidizing property on the surface layer of the high-nickel ternary material and the electrolyte have serious side reactions, so that the polarization of the battery is increased, and the capacity of the battery is quickly attenuated. And the side reaction is intensified at high temperature, which causes high-temperature storage and high-temperature cycle inflation of the battery and performance deterioration. From the commercial application of the current electrolyte, the ethylene sulfate can remarkably improve the high-temperature storage and high-temperature cycle performance of the battery, and is an additive with the best application effect in sulfate compounds, but the ethylene sulfate is high in cost, and the low-temperature storage requirement of the ethylene sulfate causes inconvenience to the transportation and storage of the electrolyte. And the improvement effect of the high-temperature additive on high-temperature storage and high-temperature circulation is not as good as that of a sulfonate additive, and the high-temperature additive which is most widely applied at present is still Propane Sultone (PS) with the best comprehensive performance. However, the use of PS is prohibited in some countries due to the disadvantages of the PS such as high harm to the body. The Chinese patent CN 106099183 adopts Pyridine Propane Sulfonate (PPS) to replace PS to ensure the cycle performance and the high-temperature performance of the battery, but the low-temperature performance of the battery cannot be effectively improved, and experiments prove that the effect of the PPS on the high-temperature improvement is not as good as that of the PS. Therefore, the development of an electrolyte system which is suitable for a silicon-based negative electrode and a high-nickel positive electrode electric core system and can simultaneously give consideration to high and low temperature performances is a technical problem to be solved urgently in the industry at present.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a lithium battery electrolyte and a lithium ion battery.
In order to achieve the purpose, the invention adopts the following technical scheme:
the lithium battery electrolyte comprises an organic solvent, a lithium salt and an additive, wherein the additive comprises fluoroethylene carbonate and one or more than two of propane sulfonate pyridinium salt, dopamine, lithium difluoro oxalate borate and lithium difluoro phosphate.
Preferably, in the lithium battery electrolyte, the additive is selected from any one of the following:
(1) fluoroethylene carbonate, pyridinium propane sulfonate and dopamine;
(2) fluoroethylene carbonate, lithium difluorooxalato borate and lithium difluorophosphate.
Preferably, in the lithium battery electrolyte, the additive further includes tris (trimethylsilane) borate, and more preferably, the additive includes fluoroethylene carbonate, tris (trimethylsilane) borate, pyridinium propanesulfonate, dopamine, lithium difluorooxalato borate, and lithium difluorophosphate.
Preferably, in the lithium battery electrolyte, the mass of the additive is 3 to 10%, more preferably 3 to 6%, of the mass of the lithium battery electrolyte.
Preferably, in the lithium battery electrolyte, the organic solvent includes ethyl acetate and one or more selected from ethylene carbonate, propylene carbonate, ethyl methyl carbonate and diethyl carbonate.
Preferably, in the above lithium battery electrolyte, the organic solvent includes ethyl acetate, ethylene carbonate, propylene carbonate, ethyl methyl carbonate, and diethyl carbonate.
Preferably, in the electrolyte for lithium battery, the solubility of the lithium salt in the electrolyte is 0.8-1.4 mol/L.
Preferably, in the above lithium battery electrolyte, the lithium salt includes lithium hexafluorophosphate and lithium bis-fluorosulfonylimide, and more preferably, the solubility of the lithium hexafluorophosphate in the electrolyte is 1.0mol/L, and the solubility of the lithium bis-fluorosulfonylimide in the electrolyte is 0.1 mol/L.
The invention also provides a lithium ion battery, which comprises a positive plate, a negative plate, a diaphragm and the electrolyte, wherein the electrolyte is the lithium battery electrolyte.
Preferably, in the lithium ion battery, the positive plate includes an aluminum current collector and a positive coating including a high-nickel positive active material, a first conductive agent and a first binder coated on the aluminum current collector, the negative plate includes a copper current collector and a negative coating including a silicon-based negative active material, a second conductive agent and a second binder coated on the copper current collector, and the separator is a polyolefin separator.
The invention has the following beneficial effects:
the invention provides a wide-temperature electrolyte which is suitable for silicon-based negative electrodes and high-nickel positive lithium ion batteries and does not generate harmful substances to human bodies, and a high-specific-energy lithium ion battery adopting the electrolyte. The electrolyte utilizes the synergistic effect of pyridinium propanesulfonate, dopamine, lithium difluoro-oxalato-borate and lithium difluoro-phosphate to replace the traditional propane sultone, improves the high-temperature storage and high-temperature cycle performance of the battery, greatly improves the low-temperature discharge capacity, and does not generate harmful substances; and simultaneously, the wettability of the electrolyte to an electrode material and a diaphragm is improved under a low-temperature condition by adopting ethyl acetate.
Detailed Description
The present invention will be described in further detail with reference to specific examples, but the scope of the present invention is not limited thereto.
In the following examples and comparative examples, the purity of the lithium salt used is 99.9% or more, the purity of the organic solvent is 99.98% or more, the purity of the additive is 99.9% or more, and the abbreviations for the respective substances are as follows:
ethylene carbonate EC, propylene carbonate PC, ethylmethyl carbonate EMC, diethyl carbonate DEC, ethyl acetate EP, dimethyl carbonate DMC, lithium LiFSI, lithium hexafluorophosphate LiPF6Fluoroethylene carbonate FEC, tris (trimethylsilane) borate TMSB, pyridinium propanesulfonate PPS, lithium difluorooxalato borate LiDFOB, lithium difluorophosphate LiPO2F2Propane sultone PS, N-methylpyrrolidone NMP.
Example 1
1. Preparation of lithium battery electrolyte
In the examples, the electrolyte was prepared in an argon glove box in which the water content and oxygen content were controlled to 0.5ppm or less, and a lithium battery electrolyte was prepared by adding 3% by mass of fluoroethylene carbonate, 0.5% by mass of pyridinium propanesulfonate and 0.1% by mass of dopamine to a solution of lithium hexafluorophosphate (concentration 1mol/L) and lithium bis (fluorosulfonylimide) (concentration 0.1mol/L) of ethylene carbonate, propylene carbonate, ethyl methyl carbonate, diethyl carbonate, ethyl acetate (EC: PC: DEC: EMC: EP ═ 15:5:10:65: 5). The detection shows that the electrolyte water content is less than 20PPM and the free acid is less than 50 PPM.
2. Preparation of positive and negative electrodes
Preparing a high nickel electrode sheet: uniformly mixing a high-nickel positive electrode active substance (NCM811), conductive carbon black Super-P and a PVDF binder according to a mass ratio of 90:6:4, adding a proper amount of NMP to adjust viscosity, and uniformly mixing the components to obtain slurry. The slurry was then uniformly coated on aluminum foil with an automatic coater and rolled for use.
Preparing a silicon-carbon negative electrode: uniformly mixing a silicon-carbon negative electrode active substance (the silicon content is 7%), conductive carbon black Super-P, a carboxymethylcellulose sodium CMC binder and a styrene butadiene rubber SBR binder according to the mass ratio of 91:5:2:2, adding a proper amount of deionized water to adjust the viscosity, and uniformly mixing the components to obtain the slurry. And then uniformly coating the slurry on the copper foil by using an automatic coating machine, and rolling for later use.
3. Preparation of lithium ion battery
In the preparation of the 2Ah lithium ion battery in this embodiment, a high nickel electrode plate is used as a positive electrode, a silicon carbon electrode plate is used as a negative electrode, a polyolefin diaphragm (a star source material SD220202) and the electrolyte prepared in step 1 are used, assembly is completed in a high-purity argon (99.99%) glove box with the moisture content and the oxygen content both lower than 0.5ppm, pre-charging is performed (pre-charging is performed for 5 hours at a constant current of 0.1C, charging is performed to 4.2V at a constant current and constant voltage of 0.1C, then charging and discharging are performed for 2 weeks at a charging cut-off voltage of 4.2V and a discharging cut-off voltage of 2.8V, charging is performed at a constant current and constant voltage, discharging is performed at a constant current.
Example 2
A lithium ion battery was prepared according to the method of example 1, except that the organic solvent in the electrolyte used was ethylene carbonate, propylene carbonate, ethyl methyl carbonate, dimethyl carbonate, diethyl carbonate (EC: PC: DEC: EMC: DMC: EP: 15:5:10:35:30: 5).
Example 3
A lithium ion battery was prepared according to the method of example 1, except that the organic solvent in the electrolyte was ethylene carbonate, propylene carbonate, ethyl methyl carbonate, diethyl carbonate (EC: PC: DEC: EMC ═ 15:5:10: 70).
Example 4
A lithium ion battery was fabricated in accordance with the procedure of example 1, except that the electrolyte was used with additives of 3% fluoroethylene carbonate, 0.5% lithium difluorooxalato borate and 1% lithium difluorophosphate, respectively, by mass ratio.
Example 5
A lithium ion battery was prepared according to the method of example 1, except that the electrolyte was used with additives of fluoroethylene carbonate 3%, tris (trimethylsilane) borate 1%, pyridinium propane sulfonate 0.5% and dopamine 0.1% by mass, respectively.
Example 6
A lithium ion battery was prepared in accordance with the method of example 1, except that the electrolyte was used with additives of 3% fluoroethylene carbonate, 1% tris (trimethylsilane) borate, 0.5% lithium difluorooxalato borate and 1% lithium difluorophosphate, respectively, by mass ratio.
Example 7
A lithium ion battery was prepared in accordance with the method of example 1, except that the electrolyte was used with additives of 3% fluoroethylene carbonate, 1% tris (trimethylsilane) borate, 0.5% pyridinium propanesulfonate, 0.1% dopamine, 0.5% lithium difluorooxalato borate and 1% lithium difluorophosphate, respectively, by mass.
Comparative example 1
A lithium ion battery was fabricated in accordance with the method of example 1, except that the electrolyte was used with additives of fluoroethylene carbonate and propane sultone in the mass ratios of 3% and 3%, respectively.
Test examples
The lithium ion batteries prepared in examples 1 to 7 and comparative example 1 were charged at constant current and constant voltage, and were discharged at constant current with a charge cut-off voltage of 4.2V and a discharge cut-off voltage of 2.8V, and the results of the charge and discharge tests were performed at a 1C rate, as shown in table 1. The discharge capacity of the battery after storage or cyclic charge and discharge is defined as the retention capacity, and the discharge capacity of the battery after charge is defined as the recovery capacity, where the capacity retention rate is the retention capacity/initial discharge capacity × 100% of the battery, and the capacity recovery rate is the recovery capacity/initial discharge capacity × 100% of the battery.
Table 1 comparison of charge and discharge test results for lithium ion batteries of examples and comparative examples
As can be seen from table 1, the batteries prepared using the electrolyte of the present invention have greatly improved low-temperature discharge capacity while improving high-temperature storage and high-temperature cycle performance.
Although the invention has been described in detail hereinabove by way of general description, specific embodiments and experiments, it will be apparent to those skilled in the art that many modifications and improvements can be made thereto based on the invention. Accordingly, such modifications and improvements are intended to be within the scope of the invention as claimed.
Claims (12)
1. A lithium battery electrolyte comprising an organic solvent, a lithium salt and an additive, wherein the additive comprises fluoroethylene carbonate, pyridinium propanesulfonate, dopamine, lithium difluorooxalato borate and lithium difluorophosphate.
2. The lithium battery electrolyte of claim 1, wherein the additive further comprises tris (trimethylsilane) borate.
3. The lithium battery electrolyte as claimed in claim 1 or 2, wherein the mass of the additive is 3-10% of the mass of the lithium battery electrolyte.
4. A lithium battery electrolyte as claimed in claim 3, wherein the mass of the additive is 3-6% of the mass of the lithium battery electrolyte.
5. The lithium battery electrolyte as claimed in claim 1 or 2, wherein the organic solvent includes ethyl acetate and one or more selected from ethylene carbonate, propylene carbonate, ethyl methyl carbonate, and diethyl carbonate.
6. The lithium battery electrolyte of claim 5, wherein the organic solvent comprises ethyl acetate, ethylene carbonate, propylene carbonate, ethyl methyl carbonate, and diethyl carbonate.
7. The lithium battery electrolyte as claimed in claim 1 or 2, wherein the solubility of the lithium salt in the electrolyte is 0.8 to 1.4 mol/L.
8. A lithium battery electrolyte as claimed in claim 1 or 2, wherein the lithium salt comprises lithium hexafluorophosphate and lithium bis-fluorosulfonylimide.
9. The lithium battery electrolyte of claim 7, wherein the lithium salt comprises lithium hexafluorophosphate and lithium bis-fluorosulfonylimide.
10. The lithium battery electrolyte as claimed in claim 8, wherein the solubility of the lithium hexafluorophosphate in the electrolyte is 1.0mol/L and the solubility of the lithium bis-fluorosulfonylimide in the electrolyte is 0.1 mol/L.
11. A lithium ion battery comprising a positive electrode sheet, a negative electrode sheet, a separator and an electrolyte, wherein the electrolyte is the lithium battery electrolyte according to any one of claims 1 to 10.
12. The lithium ion battery according to claim 11, wherein the positive plate comprises an aluminum current collector and a positive coating coated on the aluminum current collector and comprising a high nickel positive active material, a first conductive agent and a first binder, the negative plate comprises a copper current collector and a negative coating coated on the copper current collector and comprising a silicon-based negative active material, a second conductive agent and a second binder, and the separator is a polyolefin separator.
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CN111934009B (en) * | 2020-07-14 | 2021-12-03 | 华中科技大学 | High-voltage-resistant quick-charging lithium ion battery electrolyte and preparation method and application thereof |
CN112054241B (en) * | 2020-10-15 | 2022-06-21 | 广州天赐高新材料股份有限公司 | Fluorine-containing sulfonate electrolyte additive, electrolyte containing additive and lithium ion battery |
CN112838272A (en) * | 2021-01-05 | 2021-05-25 | 浙江南都电源动力股份有限公司 | Electrolyte for low-temperature lithium ion battery and lithium ion battery |
CN113206297B (en) * | 2021-05-07 | 2022-07-29 | 徐文忠 | Multifunctional composite electrolyte additive |
CN115602922A (en) * | 2022-10-24 | 2023-01-13 | 江西远东电池有限公司(Cn) | High-nickel silicon-based lithium ion battery electrolyte and cylindrical high-nickel silicon-based lithium ion battery |
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