CN110797572B - Lithium ion battery electrolyte and lithium ion battery - Google Patents
Lithium ion battery electrolyte and lithium ion battery Download PDFInfo
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- CN110797572B CN110797572B CN201810876103.2A CN201810876103A CN110797572B CN 110797572 B CN110797572 B CN 110797572B CN 201810876103 A CN201810876103 A CN 201810876103A CN 110797572 B CN110797572 B CN 110797572B
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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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- 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
In order to overcome the problems of insufficient overcharge resistance and low-temperature discharge performance of the conventional lithium ion battery, the invention provides a lithium ion battery electrolyte, which comprises a solvent, a lithium salt, 2-dicyanovinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylenedioxythiophene. Meanwhile, the invention also discloses a lithium ion battery comprising the electrolyte. The lithium ion battery electrolyte provided by the invention can well improve the overcharge resistance and low-temperature discharge performance of the battery.
Description
Technical Field
The invention belongs to the technical field of secondary batteries, and particularly relates to a lithium ion battery electrolyte and a lithium ion battery.
Background
The lithium ion battery has the remarkable advantages of high specific energy, large specific power, long cycle life, small self-discharge and the like, is popular with consumers, and is widely applied to 3C electronic products and power batteries such as mobile communication, digital cameras, video cameras and the like. With the daily wide application of lithium ion batteries, various electronic devices have higher requirements on the safety performance of the lithium ion batteries.
Safety is the most basic requirement of the lithium ion battery, in a safety test, overcharge resistance is one of safety performance, and at present, overcharge and ignition are one of the main problems encountered by the lithium ion battery.
Secondly, the performance of low-temperature discharge is very important to the application range of the lithium ion battery, and good low-temperature discharge performance is used for solving the daily use problem of users in alpine regions.
Disclosure of Invention
The invention provides a lithium ion battery electrolyte and a lithium ion battery, aiming at the problem that the existing lithium ion battery has insufficient overcharge resistance and low-temperature discharge performance.
The technical scheme adopted by the invention for solving the technical problems is as follows:
in one aspect, an embodiment of the present invention provides an electrolyte for a lithium ion battery, including a solvent, a lithium salt, 2-dicyanovinyl-4-vinyl-1, 3-dioxolane, and 3, 4-ethylenedioxythiophene.
The invention provides a lithium ion battery electrolyte, which is added with 2-dicyano vinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylene dioxythiophene as additives, and the inventor finds that compared with the single addition of 2-dicyano vinyl-4-vinyl-1, 3-dioxolane or 3, 4-ethylene dioxythiophene in the electrolyte, the combination of 2-dicyano vinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylene dioxythiophene in the electrolyte improves the stability of the electrolyte, can absorb internal electrons to reduce the reaction heat when a battery core is overcharged, reduces the decomposition of the electrolyte at high temperature and reduces the generation of gas; meanwhile, a stable SEI film is formed on the positive electrode and the negative electrode, so that the low-temperature discharge performance of the lithium ion battery is effectively improved.
Optionally, the mass percentage content of the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane in the electrolyte is 0.1-5%.
Optionally, the 3, 4-ethylenedioxythiophene accounts for 0.1-5% of the electrolyte by mass.
Optionally, the concentration of the lithium salt in the electrolyte is 0.5M to 2M.
Optionally, the lithium salt includes one or more of an organic lithium salt and an inorganic lithium salt.
Optionally, the lithium salt comprises one or more of hexafluorophosphate, hexafluoroarsenate, perchlorate, lithium trifluorosulfonyl, lithium bis (trifluoromethylsulfonyl) imide, lithium bis (fluorosulfonyl) imide and lithium tris (trifluoromethylsulfonyl) methide.
Optionally, the solvent is two or more selected from ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl formate, ethyl propionate, propyl propionate, methyl butyrate and tetrahydrofuran.
Optionally, the electrolyte is composed of a solvent, a lithium salt, 2-dicyanovinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylenedioxythiophene.
On the other hand, another embodiment of the invention discloses a lithium ion battery, which comprises a positive plate, a negative plate, a diaphragm and the electrolyte.
The lithium ion battery provided by the invention has better overcharge resistance and low-temperature discharge performance due to the adoption of the electrolyte.
Optionally, the positive plate includes a positive active material, and the positive active material includes one or more of a lithium cobaltate, a lithium nickel cobalt manganese, and lithium iron phosphate and lithium manganate.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects solved by the present invention more apparent, the present invention is further described in detail below with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The embodiment of the invention discloses a lithium ion battery electrolyte, which comprises a solvent, lithium salt, 2-dicyano vinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylene dioxythiophene.
The chemical structural formula of the 2-dicyano vinyl-4-vinyl-1, 3-dioxolane is shown as follows:
the chemical structural formula of the 3, 4-ethylenedioxythiophene is as follows:
the inventor finds that, compared with the independent addition of 2-dicyanovinyl-4-vinyl-1, 3-dioxolane or 3, 4-ethylenedioxythiophene in the electrolyte, the combination of 2-dicyanovinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylenedioxythiophene in the electrolyte improves the stability of the electrolyte, can absorb internal electrons to reduce reaction heat when a battery core is overcharged, reduces decomposition of the electrolyte at high temperature, and reduces gas generation; meanwhile, a stable SEI film is formed on the positive electrode and the negative electrode, so that the low-temperature discharge performance of the lithium ion battery is effectively improved.
In some embodiments, the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane is present in the electrolyte in an amount of 0.1 to 5% by weight.
When the mass percentage content of the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane in the electrolyte is less than 0.1 percent, the electrolyte can not play a role of a high-voltage additive; when the mass percentage content is higher than 5%, a compact passive film is easily formed on the positive electrode and the negative electrode to increase the impedance, and the conductivity and the cycle performance of the battery are influenced.
When the mass percentage of the 3, 4-ethylenedioxythiophene in the additive is less than 0.1%, the film forming effect of the electrolyte on the electrode is not ideal, and the improvement effect on the low-temperature discharge performance is not obvious; above 5%, the battery is liable to store swelling and increase in resistance at high temperatures.
In some preferred embodiments, the 3, 4-ethylenedioxythiophene accounts for 0.1-3% of the electrolyte by mass. Further preferably, the upper limit of the content range of the 3, 4-ethylenedioxythiophene in the electrolyte is selected from 5% and 3%, and the lower limit is selected from 0.1%, 0.2% and 0.5%.
In some preferred embodiments, the content of the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane in the electrolyte solution is in a mass percentage range with an upper limit selected from 5% and a lower limit selected from 0.1% and 0.2%.
Still more preferably, the 3, 4-ethylenedioxythiophene accounts for 3 to 5 mass percent of the electrolyte, the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane accounts for 0.2 to 3 mass percent of the electrolyte, and when the content ratio of the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane to the 3, 4-ethylenedioxythiophene is within the above range, the electrolyte has the best high-temperature stability and low-temperature discharge effect.
The amount of the lithium salt may vary over a wide range, and in some embodiments, the concentration of the lithium salt in the electrolyte is 0.5M to 2M. When the concentration of the lithium salt is too low, the conductivity of the electrolyte is low, and the multiplying power and the cycle performance of the whole battery system can be influenced; when the concentration of the lithium salt is too high, the viscosity of the electrolyte is too high, which is also not beneficial to the improvement of the rate of the whole battery system. In a more preferred embodiment, the lithium salt concentration is 0.9M to 1.3M.
In some embodiments, the lithium salt includes one or more of an organic lithium salt and an inorganic lithium salt.
For example: LiPF6，LiBF4，LiSbF6，LiAsF6，LiTaF6，LiAlCl4，Li2B10Cl10，Li2B10F10，LiClO4，LiCF3SO3Salts of lithium chelated orthoborates and chelated orthophosphates, e.g. lithium bis (oxalato) borate [ LiB (C)2O4)2]Lithium dimalonate borate [ LiB (O)2CCH2CO2)2]Lithium bis (difluoromalonate) borate [ LiB (O)2CCF2CO2)2](malonic acid oxalic acid) lithium borate [ LiB (C)2O4)(O2CCH2CO2)]Lithium (difluoromalonic acid oxalic acid) borate [ LiB (C)2O4)(O2CCF2CO2)]Lithium tris (oxalato) phosphate [ LiP (C)2O4)3]And lithium tris (difluoromalonate) phosphate [ LiP (O)2CCF2CO2)3]And any combination of two or more of the foregoing lithium salts.
In some embodiments, the lithium salt is selected from lithium fluoride salts.
In preferred embodiments, the lithium salt comprises one or more of hexafluorophosphate, hexafluoroarsenate, perchlorate, lithium trifluorosulfonyl, lithium bis (trifluoromethylsulfonyl) imide, lithium bis (fluorosulfonyl) imide and lithium tris (trifluoromethylsulfonyl) methide.
In some embodiments, the solvent is selected from non-aqueous organic solvents.
In a preferred embodiment, the solvent is selected from two or more of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl formate, ethyl propionate, propyl propionate, methyl butyrate and tetrahydrofuran.
In some embodiments, the electrolyte solution further includes other additives for promoting the formation of the SEI film, and specifically, the additives include, but are not limited to: vinylene carbonate and its derivatives, ethylene carbonate derivatives having non-conjugated unsaturated bonds in the side chain thereof, cyclic carbonates substituted with halogen, and salts of chelate orthoborates and chelate orthophosphoric esters.
Specifically, the additive comprises one or more of vinylene carbonate, ethylene carbonate, methylene ethylene carbonate, fluoroethylene carbonate, trifluoromethyl ethylene carbonate and difluoroethylene carbonate.
In one embodiment, the electrolyte is composed of a solvent, a lithium salt, 2-dicyanovinyl-4-vinyl-1, 3-dioxolane, and 3, 4-ethylenedioxythiophene.
Another embodiment of the present invention provides a lithium ion battery, including a positive electrode sheet, a negative electrode sheet, a separator, and the electrolyte as described above.
The positive plate comprises a positive active material, wherein the positive active material comprises one or more of lithium cobaltate, nickel cobalt manganese lithium ternary material, lithium iron phosphate and lithium manganate. Preferably, the positive electrode material is lithium cobaltate or a nickel cobalt manganese lithium ternary material.
The positive plate also comprises a positive current collector for leading out current, and the positive active material is mixed with the binder, the conductive agent and the solution, then coated on the positive current collector and dried to form the positive plate.
The negative plate comprises a negative current collector and a negative active material coated on the negative current collector, wherein the negative active material is mixed with a binder, a conductive agent and a solution and then coated on the negative current collector and dried to form the negative plate.
The negative active material includes one or more of a carbon material, a metal alloy, a lithium-containing oxide, and a silicon-containing material.
In a preferred embodiment, the negative active material is selected from graphite.
The upper limit charging voltage of the lithium ion battery is 4.5V.
The lithium ion battery provided by the embodiment of the invention can absorb internal electrons to reduce reaction heat when a battery core is overcharged due to the electrolyte, and simultaneously forms a stable SEI film on a positive electrode and a negative electrode, thereby effectively improving low-temperature discharge performance.
The present invention will be further illustrated by the following examples.
Example 1
The embodiment is used for explaining the lithium ion battery electrolyte, the lithium ion battery and the preparation method thereof, and the preparation method comprises the following operation steps:
preparing an electrolyte: EC, DEC, PC were mixed at 1: 1: 1 as an organic solvent. Adding the additive with the mass percentage content shown in the example 1 in the table 1 into the organic solvent, uniformly mixing, and adding LiPF6Obtaining LiPF6Electrolyte with the concentration of 1.1 mol/L.
Manufacturing a positive plate: the positive electrode active material lithium cobaltate (LiCoO)2) The conductive agent CNT (Carbon nano tube) and the adhesive polyvinylidene fluoride are fully stirred and mixed in the N-methyl pyrrolidone solvent according to the weight ratio of 97:1.5:1.5, so that uniform anode slurry is formed. And coating the slurry on an Al foil of a positive current collector, drying and cold pressing to obtain the positive plate.
And (3) manufacturing a negative plate: the negative electrode active material graphite, the conductive agent acetylene black, the binder styrene butadiene rubber and the thickener sodium carboxymethyl cellulose are fully stirred and mixed in a proper amount of deionized water solvent according to the mass ratio of 95:2:2:1 to form uniform negative electrode slurry. And coating the slurry on a Cu foil of a negative current collector, drying and cold pressing to obtain the negative plate.
Manufacturing the lithium ion battery: the PE porous polymer film is used as a separation film.
The positive pole piece, the isolating membrane and the negative pole piece are sequentially stacked, so that the isolating membrane is positioned between the positive pole and the negative pole, the isolating effect is achieved, and then the bare cell can be wound. And placing the bare cell into an outer packaging bag, respectively injecting the prepared electrolyte into the dried battery, and performing vacuum packaging, standing, formation, shaping and other processes to complete the preparation of the lithium ion battery.
Examples 2 to 8
Examples 2 to 8 are provided to illustrate the lithium ion battery electrolyte, the lithium ion battery and the preparation method thereof disclosed in the present invention, including most of the operation steps as in example 1, and the differences are as follows:
in the preparation operation of the electrolyte: the additive with the mass percentage content shown in the embodiment 2-8 in the table 1 is added into the organic solvent.
Comparative examples 1 to 3
Comparative examples 1 to 3 are provided for comparative illustration of the lithium ion battery electrolyte, the lithium ion battery and the preparation method thereof disclosed in the present invention, including most of the operation steps as in example 1, and the differences are as follows:
in the preparation operation of the electrolyte: the additive with the mass percentage content shown in comparative examples 1-3 in the table 1 is added into the organic solvent.
Performance testing
The lithium ion batteries prepared in the above examples 1 to 8 and comparative examples 1 to 3 were subjected to the following performance tests:
anti-overcharge test of the battery: the battery in a semi-charging state is discharged to 3.0V at the temperature of 25 ℃ at the temperature of 0.5C, then is charged to 10V at the constant current of 0.5C, and then is charged for 2 hours at the constant current of 10V, and meanwhile, the temperature change of the battery in the charging process is tested and the state of the battery after the test is observed.
The battery is not ignited and not exploded, and the surface temperature rise is lower than 150 ℃, which is considered to be passed.
Low temperature testing of the battery: discharging the semi-electric battery to 3.0V at 25 deg.C at 0.5C, charging and discharging at 0.5C once to record initial capacity, standing at-30 deg.C for 4 hr until the battery is cooled, discharging at 0.3C to 3.0V, and recording discharge capacity.
Capacity retention (%) low temperature discharge capacity (mAh)/initial capacity (mAh) × 100%
The test results obtained are filled in Table 1.
TABLE 1
From the test results in table 1, it can be seen that, compared with comparative examples 1 to 3, the overcharge resistance and the low-temperature discharge resistance of the battery cell prepared in examples 1 to 8 of the technical scheme of the present application are significantly improved.
The test results of the comparative examples 1 and 2 and the examples 3 to 8 show that in the preferable content range of the present application, the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylenedioxythiophene have a better combination effect, and the overcharge resistance and the low-temperature discharge resistance are reduced to a certain extent when the content is beyond the range.
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 (10)
1. The lithium ion battery electrolyte is characterized by comprising a solvent, lithium salt, 2-dicyanovinyl-4-vinyl-1, 3-dioxolane and 3, 4-ethylenedioxythiophene.
2. The lithium ion battery electrolyte of claim 1, wherein the 2-dicyanovinyl-4-vinyl-1, 3-dioxolane is present in the electrolyte in an amount of 0.1-5% by weight.
3. The lithium ion battery electrolyte of claim 1, wherein the 3, 4-ethylenedioxythiophene is present in the electrolyte in an amount of 0.1-5% by weight.
4. The lithium ion battery electrolyte of claim 1, wherein the concentration of the lithium salt in the electrolyte is between 0.5M and 2M.
5. The lithium ion battery electrolyte of claim 1, wherein the lithium salt comprises one or more of an organic lithium salt and an inorganic lithium salt.
6. The lithium ion battery electrolyte of claim 1, wherein the lithium salt comprises one or more of hexafluorophosphate, hexafluoroarsenate, perchlorate, lithium trifluorosulfonyl, lithium bis (trifluoromethylsulfonyl) imide, lithium bis (fluorosulfonyl) imide, and lithium tris (trifluoromethylsulfonyl) methide.
7. The lithium ion battery electrolyte of claim 1, wherein the solvent is selected from two or more of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl formate, ethyl propionate, propyl propionate, methyl butyrate, and tetrahydrofuran.
8. The lithium ion battery electrolyte of claim 1, wherein the electrolyte is comprised of a solvent, a lithium salt, 2-dicyanovinyl-4-vinyl-1, 3-dioxolane, and 3, 4-ethylenedioxythiophene.
9. A lithium ion battery comprising a positive electrode sheet, a negative electrode sheet, a separator and the electrolyte according to any one of claims 1 to 8.
10. The lithium ion battery of claim 9, wherein the positive plate comprises a positive active material comprising one or more of lithium cobaltate, lithium nickel cobalt manganese, lithium iron phosphate and lithium manganese.
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| CN104577200A (en) * | 2015-02-06 | 2015-04-29 | 宁德新能源科技有限公司 | Electrolyte additive and application thereof |
| CN105229090A (en) * | 2013-05-31 | 2016-01-06 | 3M创新有限公司 | LBL self assembly comprises method and the goods of the polymer electrolyte of photoabsorption or Photostabilised compound |
| CN105826606A (en) * | 2016-05-16 | 2016-08-03 | 宁德时代新能源科技股份有限公司 | Electrolyte and lithium ion battery containing same |
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| US8288040B2 (en) * | 2009-02-17 | 2012-10-16 | Toyota Motor Engineering & Manufacturing North America, Inc. | High voltage electrolyte |
| CN102709589B (en) * | 2012-02-17 | 2016-04-13 | 深圳新宙邦科技股份有限公司 | Lithium ion battery and electrolyte thereof |
| CN107845832A (en) * | 2017-10-27 | 2018-03-27 | 山东大学 | A kind of non-flammable lithium-ion battery electrolytes of Low ESR and preparation method thereof |
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| CN105229090A (en) * | 2013-05-31 | 2016-01-06 | 3M创新有限公司 | LBL self assembly comprises method and the goods of the polymer electrolyte of photoabsorption or Photostabilised compound |
| CN104577200A (en) * | 2015-02-06 | 2015-04-29 | 宁德新能源科技有限公司 | Electrolyte additive and application thereof |
| CN105826606A (en) * | 2016-05-16 | 2016-08-03 | 宁德时代新能源科技股份有限公司 | Electrolyte and lithium ion battery containing same |
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