CN111653829A - Lithium ion battery electrolyte and lithium ion battery - Google Patents
Lithium ion battery electrolyte and lithium ion battery Download PDFInfo
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- CN111653829A CN111653829A CN202010697235.6A CN202010697235A CN111653829A CN 111653829 A CN111653829 A CN 111653829A CN 202010697235 A CN202010697235 A CN 202010697235A CN 111653829 A CN111653829 A CN 111653829A
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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
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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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
- H01M2220/00—Batteries for particular applications
- H01M2220/30—Batteries in portable systems, e.g. mobile phone, laptop
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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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- 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
- H01M2300/0088—Composites
- H01M2300/0091—Composites in the form of mixtures
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
Disclosed is a lithium ion battery electrolyte, which comprises a film forming additive, wherein the film forming additive comprises vinylene carbonate, vinyl sulfate, 1, 3-propane sultone and lithium difluorophosphate; vinylene carbonate accounts for 0.2-3% of the total mass of the electrolyte, vinyl sulfate accounts for 0.5-5% of the total mass of the electrolyte, 1, 3-propane sultone accounts for 0.2-3% of the total mass of the electrolyte, and lithium difluorophosphate accounts for 0.2-2% of the total mass of the electrolyte. In the electrolyte, vinylene carbonate and vinyl sulfate form a stable and compact SEI film on the surface of a battery cathode in the formation and charge-discharge processes, and 1, 3-propane sultone and lithium difluorophosphate form a passivation film on the surface of a cathode, so that the high-temperature gas production performance of the battery is improved, the damage of cathode transition metal element dissolution in the rapid charge cycle process to the cathode is inhibited, the film forming structure of the cathode and the anode is improved, side reactions are reduced, and the battery is ensured to have good high-rate charge performance and cycle life.
Description
Technical Field
The invention belongs to the field of lithium ion batteries, and particularly relates to a lithium ion battery electrolyte and a lithium ion battery containing the same.
Background
In recent years, lithium ion batteries have been widely used in the fields of smart phones, tablet computers, smart wearing, electric tools, electric automobiles, and the like. With the acceleration of life rhythm and the development of electronic products, consumers have more urgent needs for shortening the charging time of the lithium ion battery and improving the energy density of the lithium ion battery, and correspondingly, higher requirements are put forward on the charging speed of the lithium ion battery.
At present, the requirement of quick charging is met by adding various additives into electrolyte, but the existing lithium ion battery electrolyte can cause the DCR and polarization of the battery to be larger, the situation of lithium precipitation caused by quick charging and high-rate circulation is easy to cause, and the quick charging time is difficult to shorten and the quick charging performance is difficult to improve.
Disclosure of Invention
In order to overcome the defects, the invention provides an electrolyte of a lithium ion battery and the lithium ion battery containing the electrolyte.
The invention provides an electrolyte of a lithium ion battery, which comprises a film forming additive, wherein the film forming additive comprises vinylene carbonate, vinyl sulfate, 1, 3-propane sultone and lithium difluorophosphate; the vinylene carbonate accounts for 0.2-3% of the total mass of the electrolyte, the vinyl sulfate accounts for 0.5-5% of the total mass of the electrolyte, the 1, 3-propane sultone accounts for 0.2-3% of the total mass of the electrolyte, and the lithium difluorophosphate accounts for 0.2-2% of the total mass of the electrolyte.
In another aspect, the invention provides a lithium ion battery comprising the electrolyte.
The electrolyte comprises a film forming additive, wherein a stable and compact SEI film is formed on the surface of a battery cathode in the processes of formation and charge-discharge of vinylene carbonate and vinyl sulfate, and a passivation film is formed on the surface of a cathode by 1, 3-propane sultone and lithium difluorophosphate, so that the high-temperature gas production performance of the battery is improved, and the damage of cathode transition metal element dissolution in the rapid charge cycle process to the cathode is inhibited. The electrolyte can improve the film forming structure of the positive electrode and the negative electrode and reduce side reaction through the combination of the four additives, and ensures that the battery has good high-rate charging performance and cycle life.
Detailed Description
The present invention will be described in detail with reference to the following embodiments.
The lithium ion battery electrolyte comprises a film forming additive, wherein the film forming additive comprises Vinylene Carbonate (VC), vinyl sulfate (DTD), 1, 3-Propane Sultone (PS) and lithium difluorophosphate (LiPO)2F2). Vinylene carbonate accounts for 0.2-3% of the total mass of the electrolyte, vinyl sulfate accounts for 0.5-5% of the total mass of the electrolyte, 1, 3-propane sultone accounts for 0.2-3% of the total mass of the electrolyte, and lithium difluorophosphate accounts for 0.2-2% of the total mass of the electrolyte.
In the electrolyte, vinylene carbonate and vinyl sulfate form a stable and compact SEI film on the surface of a negative electrode in the processes of formation, charging and discharging, and 1, 3-propane sultone and lithium difluorophosphate form a passivation film on the surface of a positive electrode, so that the high-temperature gas production performance of the battery is improved, and the damage of the dissolution of a positive electrode transition metal element to the negative electrode in the process of fast charging circulation is inhibited. The electrolyte can improve the film forming structure of the positive electrode and the negative electrode and reduce side reaction through the combination of the four additives, and ensures that the battery has good high-rate charging performance and cycle life.
In an optional embodiment, the electrolyte further comprises a low-impedance additive, so that the thickness and compactness of the SEI film can be further optimized, the interface impedance of the battery is reduced, and the quick charge performance and the normal-temperature cycle performance are obviously improved. The low impedance additive is selected from one or more of tris (trimethylsilane) borate (TMSB), tris (trimethylsilane) phosphate (TMSP), tris (trimethylsilane) phosphite (TMSPI), Methylene Methanedisulfonate (MMDS), fluoroethylene carbonate (FEC). The low-impedance additive TMSB/TMSP/TMSPI participates in the film formation of the negative electrode of the battery in a chemically modified mode, and the MMDS and the FEC with lower reduction potential can slow down the film formation of the additive with higher impedance in a certain range after the MMDS and the FEC with lower reduction potential preferentially form the film. One or more of the low-impedance additives are selected from the electrolyte, so that the interface impedance of the battery can be further reduced and the quick charging capacity can be improved by optimizing the structure of the positive and negative electrode interface films. Preferably, the low-impedance additive accounts for 0.2-5% of the total mass of the electrolyte.
In an optional embodiment, the electrolyte further comprises a high-temperature additive to improve the thermal stability of the electrolyte, reduce the occurrence of side reactions of a positive electrode and a negative electrode, and obviously improve the high-temperature storage performance and the high-temperature cycle performance. The high-temperature additive is selected from one or more of lithium bis (fluorosulfonyl) imide (LiFSI), lithium difluorooxalato borate (LiODFB), lithium difluorobis (oxalato) phosphate (LiODFP) and lithium tetrafluorooxalato phosphate (LiFOP). The high-temperature additive LiFSI is beneficial to improving the thermal stability of the electrolyte, and the high-temperature additive LiODFB/LiODFP/LiFOP generates redox reaction on the positive electrode and the negative electrode to form a passivation film with higher conductivity. The electrolyte can effectively inhibit the direct contact of the positive and negative electrode active materials and the electrolyte by adding one or more of the high-temperature additives so as to improve the high-temperature storage performance. Preferably, the high-temperature additive accounts for 0.2-5% of the total mass of the electrolyte.
In an alternative embodiment, both low resistance and high temperature additives may be included in the electrolyte. The low-resistance additive and the high-temperature additive are added into the combination, and the proper proportion (the preferable content range) is adjusted to obtain the combination with excellent fast-charging performance, high-temperature storage performance and cycle performance. The organic solvent of the electrolyte is cyclic carbonate and linear carbonate. The cyclic carbonate is selected from one or more of Ethylene Carbonate (EC), Propylene Carbonate (PC) and fluoroethylene carbonate (FEC). The linear carbonate is selected from one or more of dimethyl carbonate (DMC), diethyl carbonate (DEC), Ethyl Methyl Carbonate (EMC), ethyl acetate and ethyl propionate. Based on the total mass of the organic solvent being 100 percent, the content of the cyclic carbonate is 10 to 50 percent, and the content of the linear carbonate is 50 to 90 percent.
The lithium salt in the electrolyte is selected from LiClO4、LiPF6、LiBOB、LiFSI、LiTFSI、LiBF4And one or more of LiODFP, wherein the concentration of lithium salt in the electrolyte is 0.7-1.5 mol/L.
The electrolyte can obviously improve the quick charge capacity of the lithium ion battery and shorten the quick charge time. Meanwhile, the lithium ion battery has excellent normal-temperature quick charge cycle life and 45-DEG C high-temperature quick charge cycle life, and the 60-DEG C high-temperature storage performance can be improved. The cost of the electrolyte system is relatively moderate, and the electrolyte system is suitable for industrial application.
The invention also comprises a lithium ion battery comprising the electrolyte. In an alternative embodiment, the positive electrode material of the lithium ion battery comprises a ternary positive electrode material.
The inventive concept of the present invention is further illustrated by the following specific examples. In the following examples and comparative examples, all the raw materials are commercially available without specific description.
Example 1
Preparing an electrolyte:
the EC, the EMC and the DEC are mixed to form the organic solvent, wherein the EC accounts for 30 percent of the total mass of the solvent, the EMC accounts for 50 percent of the total mass of the solvent and the DEC accounts for 20 percent of the total mass of the solvent in the organic solvent by taking the total mass of the organic solvent as 100 percent. Adding lithium hexafluorophosphate into a solvent, fully mixing and dissolving, wherein the solubility of lithium salt in the solution is 1 mol/L. Then adding film forming additives VC, DTD, PS and LiPO2F2And uniformly mixing to obtain an electrolyte, wherein the mass content of VC, DTD, PS and LiPO in the electrolyte is 0.2%, 0.5%, 0.2% and 100% of the total mass of the electrolyte2F2The mass content of (A) is 0.2%.
Preparing a positive pole piece:
the LiNi with the mass fraction of 97 percent is calculated by taking the total mass of the positive electrode active material, the conductive agent and the binder as 100 percent0.5Co0.2Mn0.3O2(NCM523) and 2% of conductive agent carbon black are added into 1-methyl-9-pyrrolidone solution dissolved with 1% of PVDF by mass fraction, and the mixture is uniformly mixed to form positive electrode slurry. Coating the anode slurry on an aluminum foil, drying the aluminum foil by a drying oven, rolling and slicing to obtain an anode plate, wherein the compaction density of the anode plate is 3.4g/cm3。
Preparing a negative pole piece:
adding 96% by mass of artificial graphite into an aqueous solution in which 3% by mass of binder SBR and 1% by mass of thickener CMC are dissolved, and uniformly mixing to form negative electrode slurry, wherein the total mass of the negative electrode active material, the conductive agent and the binder is 100%. Coating the negative electrode slurry on copper foil, drying by a drying oven, rolling and slicing to obtain a negative electrode piece, wherein the compaction density of the negative electrode piece is 1.5g/cm3。
Assembling a battery:
and (3) stacking and winding the isolating film, the negative plate, the isolating film and the positive plate in sequence, putting the obtained product into an aluminum-plastic bag, drying the obtained product, injecting the electrolyte into the aluminum-plastic bag, and finally packaging, forming and fixing the volume to obtain the lithium ion battery.
Examples 2 to 10 and comparative examples 1 to 3
An electrolyte and a lithium ion battery were prepared with reference to the preparation method of example 1, wherein the components of the electrolyte and the contents thereof are shown in table 1.
The lithium ion batteries prepared in examples 1 to 10 and comparative examples 1 to 3 were subjected to a quick charge capacity test, a high temperature storage test and a quick charge cycle test. Specific test conditions are as follows.
Quick charge capability test (test of charging to 80% SOC): the lithium ion batteries prepared in examples 1-10 and comparative examples 1-3 were subjected to 2.8-4.3V charge/discharge tests at room temperature of 25 + -2 deg.C and a relative humidity of 45-75%. The testing steps comprise that firstly, 4C constant current charging is carried out until the voltage is 3.94V, 2C constant current charging is carried out until the voltage is 3.98V, 1C constant current constant voltage charging is carried out until the voltage is 4.3V, and standing is carried out for 10 min; discharging at 1C constant current to 2.8V, and standing for 10 min. The time to charge the battery to 80% SOC was measured.
And (3) high-temperature storage test: 2.8-4.3V storage test is carried out on the batteries of examples 1-10 and comparative examples 1-3 in a constant temperature oven at 60 ℃, and the test step comprises charging to 4.3V at a constant current and a constant voltage of 1C under the room temperature condition and standing for 10 min; transferring the battery into a constant-temperature oven at 60 ℃ for storage for 30 days, taking out the battery every 7 days, and standing for 5 hours at room temperature; discharging at 1C constant current to 2.8V, standing for 10min, charging at 1C constant current and constant voltage to 4.3V, and circulating for 3 times.
And (3) quick charge cycle test: carrying out 2.8-4.3V circulation test on the batteries of 1-10 and comparative examples 1-3 in a constant-temperature oven at 25 ℃, wherein the test step comprises the steps of charging to 4.3V at constant current and constant voltage of 2C, and standing for 10 min; discharging at 1C constant current to 2.8V, and standing for 10 min. The cells of examples 1-10 and comparative examples 1-3 were subjected to 2.8-4.3V cycling tests in a constant temperature oven at 45 ℃ using the same procedure as the 25 ℃ cycle.
The results of the above tests are shown in table 1.
TABLE 1
With reference to table 1, it can be seen that, in examples 1 to 4 and comparative examples 1 to 3, when vinylene carbonate accounts for 0.2% to 3% of the total mass of the electrolyte, vinyl sulfate accounts for 0.5% to 5% of the total mass of the electrolyte, 1, 3-propane sultone accounts for 0.2% to 3% of the total mass of the electrolyte, and lithium difluorophosphate accounts for 0.2% to 2% of the total mass of the electrolyte, the fast charge performance, the normal temperature retention rate, and the high temperature retention rate of the battery are all significantly improved. Particularly, when the vinylene carbonate accounts for 1.5% of the total mass of the electrolyte, the vinyl sulfate accounts for 2.5% of the total mass of the electrolyte, the 1, 3-propane sultone accounts for 1.5% of the total mass of the electrolyte, and the lithium difluorophosphate accounts for 1% of the total mass of the electrolyte, the improvement range of the quick charge performance, the normal temperature retention rate and the high temperature retention rate of the battery is the largest.
Comparing example 2 with examples 5 and 6, and examples 7 and 8 with examples 9 and 10, it can be seen that the fast charging performance of the battery is improved after the low-impedance additive is added to the electrolyte, which indicates that the impedance of the battery is actually reduced after the low-impedance additive is contained in the electrolyte, and further the internal resistance of the battery is reduced.
For example 2 and examples 7 and 8, and examples 5 and 6 and examples 9 and 10, it can be seen that the addition of the high temperature additive to the electrolyte improved the capacity retention rate at 45 ℃ and the capacity recovery rate at 60 ℃.
In conclusion, the electrolyte disclosed by the invention comprises the additives with specific contents and specific quality, so that the aims of improving the quick charge performance, the normal-temperature cycle capacity retention rate, the high-temperature cycle capacity retention rate and the high-temperature storage capacity recovery rate are fulfilled. Furthermore, the electrolyte can also comprise a low-impedance additive and/or a high-temperature additive to further reduce the impedance of the battery and/or improve the high-temperature storage and cycle stability of the battery.
The preferred embodiments of the invention disclosed above are intended to be illustrative only. The preferred embodiments are not intended to be exhaustive or to limit the invention to the precise embodiments disclosed. Obviously, many modifications and variations are possible in light of the above teaching. The embodiments were chosen and described in order to best explain the principles of the invention and the practical application, to thereby enable others skilled in the art to best utilize the invention. The invention is limited only by the claims and their full scope and equivalents.
Claims (10)
1. The lithium ion battery electrolyte comprises a film forming additive and is characterized in that,
the film forming additive comprises vinylene carbonate, vinyl sulfate, 1, 3-propane sultone and lithium difluorophosphate;
the vinylene carbonate accounts for 0.2-3% of the total mass of the electrolyte, the vinyl sulfate accounts for 0.5-5% of the total mass of the electrolyte, the 1, 3-propane sultone accounts for 0.2-3% of the total mass of the electrolyte, and the lithium difluorophosphate accounts for 0.2-2% of the total mass of the electrolyte.
2. The electrolyte of claim 1, further comprising a low impedance additive selected from one or more of tris (trimethylsilane) borate, tris (trimethylsilane) phosphate, tris (trimethylsilane) phosphite, methylene methanedisulfonate, fluoroethylene carbonate.
3. The electrolyte of claim 2, wherein the low impedance additive comprises 0.2% to 5% of the total mass of the electrolyte.
4. The electrolyte of any one of claims 1 to 3, further comprising a high temperature additive selected from one or more of lithium bis (fluorosulfonyl) imide, lithium difluorooxalato borate, lithium difluorobis-oxalato phosphate, lithium tetrafluorooxalato phosphate.
5. The electrolyte of claim 4, wherein the high temperature additive comprises 0.2% to 5% of the total mass of the electrolyte.
6. The electrolyte of claim 1, wherein the organic solvent of the electrolyte is a cyclic carbonate or a linear carbonate;
the cyclic carbonate is selected from one or more of ethylene carbonate, propylene carbonate and fluoroethylene carbonate;
the linear carbonate is selected from one or more of dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, ethyl acetate and ethyl propionate;
based on the total mass of the organic solvent being 100%, the content of the cyclic carbonate is 10% -50%, and the content of the linear carbonate is 50% -90%.
7. The electrolyte of claim 1, wherein the lithium salt of the electrolyte is selected from LiClO4、LiPF6、LiBOB、LiFSI、LiTFSI、LiBF4And LiODFP.
8. The electrolyte of claim 7, wherein the concentration of the lithium salt in the electrolyte is 0.7-1.5 mol/L.
9. A lithium ion battery comprising the electrolyte of any one of claims 1 to 8.
10. The lithium ion battery of claim 9, wherein the positive electrode material of the lithium ion battery comprises a ternary positive electrode material.
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