CN109962294B - Non-aqueous lithium ion battery electrolyte and lithium ion battery - Google Patents
Non-aqueous lithium ion battery electrolyte and lithium ion battery Download PDFInfo
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- CN109962294B CN109962294B CN201910213956.2A CN201910213956A CN109962294B CN 109962294 B CN109962294 B CN 109962294B CN 201910213956 A CN201910213956 A CN 201910213956A CN 109962294 B CN109962294 B CN 109962294B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—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
- 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
- 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 provides a nonaqueous lithium ion battery electrolyte and a lithium ion battery, wherein the nonaqueous lithium ion battery electrolyte contains an organic solvent, a lithium salt, a flame retardant additive and other additives, the flame retardant additive is boric acid lithium phosphate, and when the battery is overcharged or encounters extreme high temperature, the flame retardant additive can be decomposed to generate a phosphorus oxygen radical and a boron oxygen radical and capture a hydrogen radical or a hydrogen oxygen radical generated by the electrolyte or an electrode material, so that the flame retardant effect is achieved. The prepared lithium ion battery can form compact and stable CEI and SEI films on the interfaces of positive and negative electrode materials of the battery, and meanwhile, the flame retardant additive is a lithium salt which can improve the conductivity of the electrolyte and has no negative influence on the electrochemical performance.
Description
[ technical field ]
The invention belongs to the technical field of battery electrolyte, and particularly relates to a lithium ion battery non-aqueous electrolyte and a lithium ion battery.
[ background art ]
In recent years, the lithium ion battery technology is rapidly developed, the energy density of the battery is continuously refreshed, and new energy automobiles driven by the lithium ion battery are gradually the development direction of the automobile industry in the future. The working voltage of the battery is improved, the energy density of the battery can be further improved by adopting a light weight design of a high-nickel ternary material, a silicon-carbon negative electrode material and a battery auxiliary material, but great potential safety hazards are brought. The reason is that the electrolyte for the lithium ion battery at present mainly uses carbonate organic compounds, the boiling point and the flash point of the solvents are low, and when the battery is in a severe environment, the electrolyte is easy to generate thermal runaway and cause explosion and fire.
The addition of a flame retardant to the electrolyte is one of the ways to improve the ignition of the battery. The most studied are mainly phosphate flame retardant additives, such as triphenyl phosphate, trimethyl phosphate, tris (trifluoroethyl) phosphite, and ethoxypentafluorocyclotriphosphazene. The flame retardant can be used as a free radical trapping agent to trap free radicals generated by overheating or burning of battery materials, so that the flame retardant can play a role in flame retardance. However, these flame retardant additives of phosphate esters have a high viscosity, and when added to an electrolyte, the viscosity of the electrolyte increases and the conductivity decreases, which affects the electrochemical performance (cycle performance, rate performance, etc.) of the battery. Therefore, the research on the novel electrolyte flame-retardant additive with good flame-retardant effect and without influencing the performance of the battery has great theoretical and practical significance.
[ summary of the invention ]
In order to solve the above-mentioned problems, the present invention provides a novel lithium ion battery electrolyte capable of significantly improving the flame retardant property of the battery without affecting the electrochemical properties of the battery.
The electrolyte of the non-aqueous lithium ion battery contains an organic solvent, lithium salt, a flame-retardant additive and other additives, wherein the flame-retardant additive is lithium borate phosphate shown in a formula 1.
R in the structure of the non-aqueous lithium ion battery electrolyte and the flame retardant additive1、R2、R3、R4、R5The alkyl, alkenyl, alkynyl, halogenated alkyl, halogenated alkenyl, halogenated alkynyl, aryl or halogenated aryl groups with 1-6 carbon atoms can be the same or different.
The above non-aqueous lithium ion battery electrolyte, the organic solvent comprises one or more of Ethylene Carbonate (EC), dimethyl carbonate (DMC), Ethyl Methyl Carbonate (EMC), diethyl carbonate (DEC), Propylene Carbonate (PC), Propyl Propionate (PP), Ethyl Propionate (EP), Ethyl Acetate (EA), and fluoroethylene carbonate (FEC).
In the above nonaqueous lithium ion battery electrolyte, the other additive is one of Vinylene Carbonate (VC), fluoroethylene carbonate (FEC), vinylethylene carbonate (VEC), Ethylene Sulfite (ES), phosphate esters, and acid anhydrides.
In the non-aqueous lithium ion battery electrolyte, the lithium salt is one or more of lithium hexafluorophosphate, lithium bis (oxalato) borate, lithium difluoro bis (oxalato) phosphate, lithium tetrafluoro (oxalato) phosphate, lithium tetrafluoroborate and lithium bis (fluorosulfonyl) imide, and the preferable concentration of the electrolyte lithium salt is 0.6-1.0 mol/L.
In the non-aqueous lithium ion battery electrolyte, the addition amount of the lithium borate phosphate flame retardant additive in the electrolyte is 0.5-5%.
A lithium ion battery comprises a positive electrode, a negative electrode, a diaphragm and electrolyte, wherein the electrolyte is the nonaqueous lithium ion battery electrolyte.
The invention has the following advantages:
the flame retardant additive contains phosphate radical and borate radical, can generate phosphorus oxygen radical and boron oxygen radical, reduces the flammability of the lithium ion battery under the synergistic effect, and overcomes the negative influence caused by excessive addition of single component.
The flame retardant additive contains phosphate radical which has strong solvation effect on lithium ions, so that the conductivity of the electrolyte can be improved, and the negative influence of conductivity reduction caused by adding the flame retardant additive can be compensated.
The flame retardant additive contains borate, and can form compact and stable CEI and SEI films on the interfaces of positive and negative electrode materials of the battery, so that the electrochemical performance of the battery is ensured to be stably exerted.
[ detailed description of the invention ]
The present invention will be described in detail with reference to specific examples.
Example 1: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 3/5/2, and LiPF6The concentration of lithium salt is 0.6mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, and fluoroethylene carbonateThe content of (A) is 6% of the total weight of the electrolyte, the content of adiponitrile is 5% of the total weight of the electrolyte, the content of biphenyl is 4% of the total weight of the electrolyte, and the flame retardant additive A is 5% of the total weight of the electrolyte.
Comparative example 1: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 3/5/2, and LiPF6The concentration of the lithium salt is 0.6mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive is not contained.
Example 2: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 3/5/2, and LiPF6The concentration of the lithium salt is 0.7mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive A is 5 percent of the total weight of the electrolyte.
Comparative example 2: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 3/5/2, and LiPF6The concentration of the lithium salt is 0.7mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive is not contained.
Example 3: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 3/5/2, and LiPF6The concentration of lithium salt is 0.8mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, and the content of fluoroethylene carbonate is 4 percent of the total weight of the electrolyte6% of adiponitrile, 4% of biphenyl and 5% of flame retardant additive A, wherein the adiponitrile is 5% of the total weight of the electrolyte, the biphenyl is 4% of the total weight of the electrolyte, and the flame retardant additive A is 5% of the total weight of the electrolyte.
Comparative example 3: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 1/1/1, and LiPF6The concentration of the lithium salt is 0.8mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive is not contained.
Example 4: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 1/1/1, and LiPF6The concentration of the lithium salt is 0.6mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive A is 5 percent of the total weight of the electrolyte.
Comparative example 4: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 1/1/1, and LiPF6The concentration of the lithium salt is 0.6mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive is not contained.
Example 5: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 1/1/1, and LiPF6The concentration of lithium salt is 0.7mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, and the content of adiponitrile isThe electrolyte comprises 5% of the total weight of the electrolyte, the content of biphenyl is 4% of the total weight of the electrolyte, and the flame retardant additive A is 5% of the total weight of the electrolyte.
Comparative example 5: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 1/1/1, and LiPF6The concentration of the lithium salt is 0.7mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive is not contained.
Example 6: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 1/1/1, and LiPF6The concentration of the lithium salt is 0.8mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive A is 5 percent of the total weight of the electrolyte.
Comparative example 6: preparing electrolyte in a vacuum drying glove box with the water content less than 5ppm, wherein the organic solvent is ethylene carbonate/diethyl carbonate/propylene carbonate (mass ratio) 1/1/1, and LiPF6The concentration of the lithium salt is 0.8mol/L, the content of 1, 3-propane sultone is 4 percent of the total weight of the electrolyte, the content of fluoroethylene carbonate is 6 percent of the total weight of the electrolyte, the content of adiponitrile is 5 percent of the total weight of the electrolyte, the content of biphenyl is 4 percent of the total weight of the electrolyte, and the flame retardant additive is not contained.
The battery cell is made of the above electrolyte under the same conditions, and the battery cell is tested for safety performance under the same conditions:
| initial capacity exertion/mAh | 1C10V constant pressure overcharge 2.5H | High temperature 55 ℃ short circuit | Impact of heavy object | |
| Example 1 | 5019 | No explosion and no fire | No explosion and no fire | No explosion and no fire |
| Comparative example 1 | 5024 | On fire | On fire | On fire |
| Example 2 | 5031 | No explosion and no fire | No explosion and no fire | No explosion and no fire |
| Comparative example 2 | 5042 | Not exploding and igniting | On fire | On fire |
| Example 3 | 5041 | No explosion and no fire | No explosion and no fire | No explosion and no fire |
| Comparative example 3 | 5040 | No explosion and no fire | Not exploding and igniting | On fire |
| Example 4 | 5028 | No explosion and no fire | No explosion and no fire | No explosion and no fire |
| Comparative example 4 | 5040 | On fire | On fire | On fire |
| Example 5 | 5026 | No explosion and no fire | No explosion and no fire | No explosion and no fire |
| Comparative example 5 | 5036 | Not exploding and igniting | On fire | On fire |
| Example 6 | 5037 | No explosion and no fire | No explosion and no fire | No explosion and no fire |
| Comparative example 6 | 5041 | No explosion and no fire | Not exploding and igniting | On fire |
Note: the cell design capacity was 5000 mAh.
Through the comparison of the above tests, the following results can be obtained: the battery core prepared from the non-aqueous lithium ion battery electrolyte added with the flame retardant additive has good safety performance, and does not explode or catch fire under the conditions of 2.5H constant-pressure overcharge of 1C10V or weight impact or high-temperature 55 ℃ short circuit, so that the safety performance of the battery core can be obviously improved.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (7)
1. The non-aqueous lithium ion battery electrolyte contains an organic solvent, lithium salt, a flame-retardant additive and other additives, and is characterized in that the other additives are one of Vinylene Carbonate (VC), fluoroethylene carbonate (FEC), ethylene carbonate (VEC), Ethylene Sulfite (ES), phosphate esters and acid anhydride, the flame-retardant additive is lithium borophosphate shown in a formula 1,
formula 1.
2. The non-aqueous lithium ion battery electrolyte of claim 1 wherein R in the flame retardant additive structure1、R2、R3、R4、R5The alkyl, alkenyl, alkynyl, halogenated alkyl, halogenated alkenyl, halogenated alkynyl, aryl or halogenated aryl groups with 1-6 carbon atoms can be the same or different.
3. The non-aqueous lithium ion battery electrolyte of claim 1, wherein the lithium borate phosphate salt flame retardant additive is added in an amount of 0.5% to 5% of the electrolyte.
4. The non-aqueous lithium ion battery electrolyte of claim 1, wherein: the organic solvent comprises one or more of Ethylene Carbonate (EC), dimethyl carbonate (DMC), Ethyl Methyl Carbonate (EMC), diethyl carbonate (DEC) and Propylene Carbonate (PC), Propyl Propionate (PP), Ethyl Propionate (EP), Ethyl Acetate (EA) and fluoroethylene carbonate (FEC).
5. The non-aqueous lithium ion battery electrolyte of claim 1 wherein the lithium salt is one or more of lithium hexafluorophosphate, lithium bis (oxalato) borate, lithium difluoro (oxalato) phosphate, lithium tetrafluorooxalato phosphate, lithium tetrafluoroborate, lithium bis (fluorosulfonyl) imide.
6. The non-aqueous lithium ion battery electrolyte of claim 1 wherein the concentration of lithium salt is 0.6 to 1.0 mol/L.
7. A lithium ion battery comprising a positive electrode, a negative electrode, a separator and an electrolyte, wherein the electrolyte is the non-aqueous lithium ion battery electrolyte of any one of claims 1 to 6.
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