CN105206875A - Electrolyte for improving cycle performance of anode materials of lithium-ion batteries - Google Patents
Electrolyte for improving cycle performance of anode materials of lithium-ion batteries Download PDFInfo
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- CN105206875A CN105206875A CN201510724159.2A CN201510724159A CN105206875A CN 105206875 A CN105206875 A CN 105206875A CN 201510724159 A CN201510724159 A CN 201510724159A CN 105206875 A CN105206875 A CN 105206875A
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- cycle performance
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- ion battery
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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 discloses an electrolyte for improving cycle performance of anode materials of lithium-ion batteries. The electrolyte comprises an organic solvent, lithium salt and an additive, wherein the additive is TTFEB (tri-(2,2,2-trifluoroethyl)borate), and the organic solvent comprises cyclic carbonate and linear carbonate. The added additive, namely, the TTFEB, of the electrolyte facilitates formation of stable SEI films on anode surfaces, prevents co-embedment of solvent molecules, and inhibits further reactions of anodes and the electrolyte. Meanwhile, through addition of the TTFEB, the composition of the SEI films can be improved, inert components such as LiF, Li2O, Li2O2 and the like are promoted, film impedance is reduced, polarization is reduced, and consumption of the lithium-ions is reduced. The TTFEB has an improving effect on the SEI films of the anodes, so that the electrolyte containing the TTFEB can effectively improve the cycle performance of the anode materials, the charging and discharging efficiency and the rate capability.
Description
Technical field
The invention belongs to field of lithium ion battery, relate to a kind of electrolyte improving Carbon anode, graphite cathode, silicon-based anode and tin base cathode cycle performance.
Background technology
Along with the development of human society, the traditional fossil energy such as oil, natural gas is constantly exhausted, and people also more and more pay attention to environmental issue, the novel energy of developing green environmental protection and the efficient energy storage technology of Development of Novel extremely urgent.Lithium ion battery has that volume is little, energy density is high, operating voltage is high, has extended cycle life, environmental friendliness, memory-less effect and the advantage such as self discharge is little, is therefore widely used in portable electric appts as in mobile phone, digital camera, notebook computer.Along with the progress of science and technology, the application expanding day of lithium ion battery, the new type power energy, energy storage, national defense and military etc. all have application, simultaneously also more and more higher to the requirement of lithium ion battery.
In lithium ion battery charge and discharge process negative pole surface and interface stability to electrode cycle performance and cycle performance of battery most important.Electrode can exist in long-term cyclic process that solid electrolyte interface film constantly thickens, electrode material breaks, electrode surface analyses the series of problems such as lithium, especially in electrode surface film, inorganic salts ingredients constantly increases and plays inhibition to the lithium ion transport of electrode interface, cause cell resistance increase, cycle performance declines, high rate performance declines, and finally causes shorter battery life.
For these problems, researchers adopt serial of methods to carry out modification to material list interface, by improving the composition of electrode surface film, structure, compactness and stability etc., delay the dissolved destruction of electrode surface film, improve the cycle performance of negative material.At present, mainly realized by anticathode and electrolyte modification the modification of electrode surface film, the method complex process such as wherein, the modification of anticathode is coated, mechanical lapping, surface filming, repeatability is low, and cost is higher.Adopting suitable additive to improve the simple to operate and effect of the component of electrolyte obviously, is now widely used ameliorative way.
Summary of the invention
The object of the present invention is to provide a kind of electrolyte for improving lithium ion battery negative material cycle performance, improving its chemical property by improving negative terminal surface film, effectively suppress the decay of its capacity.
For achieving the above object, the present invention is by the following technical solutions:
For improving an electrolyte for lithium ion battery negative material cycle performance, be made up of organic solvent, lithium salts and additive, wherein: described additive content is in the electrolytic solution 0.1 ~ 5.0wt%; Described organic solvent is made up of cyclic carbonate and linear carbonates, and cyclic carbonate and linear carbonates mass ratio is in the electrolytic solution 1 ~ 5:3 ~ 7; The concentration of described lithium salts is 0.5 ~ 2.5mol/L.
In the present invention, described additive is three (2,2,2-trifluoroethyl) borate (TTFEB).TTFEB can preferentially and organic solvent in negative terminal surface reduction decomposition, contribute to forming complete, fine and close SEI film, improve the stability of SEI film, the contact of effective barrier material and electrolyte, the further reduction decomposition of suppression organic solvent.Meanwhile, TTFEB is a kind of boryl anion receptor, and boryl anion receptor is to F
-, O
2-, O
2 2-have good recognition reaction Deng anion, boron atom is with sp
2the covalent molecule that hydridization is formed, a remaining unoccupied orbital can accept external lone pair electrons as Lewis acid centers, is formed with the complex of the tetrahedral configuration of sp3 hydridization, thus TTFEB can with F
-, O
2-, O
2 2-deng anion binding, thus promote inert component LiF, Li in SEI film
2o, Li
2o
2deng the dissolving of inorganic salts, improve the composition of SEI film, effectively reduce the impedance of SEI film, be beneficial to the migration of lithium ion, and reduce the consumption of lithium ion, promote the conductivity of electrolyte, improve the cycle performance of negative material.
In the present invention, described lithium salts is lithium hexafluoro phosphate (LiPF
6), LiBF4, two trifluoromethanesulfonimide lithium, at least one in two (fluorine sulphonyl) imine lithium.As preferably, lithium hexafluoro phosphate (LiPF selected by lithium salts
6), LiPF
6conductivity is high, mature preparation process, is current the most widely used lithium salts.
In the present invention, described cyclic carbonate is one or both in ethylene carbonate (EC) or fluorinated ethylene carbonate, and linear carbonates is at least one or several in diethyl carbonate (DEC), dimethyl carbonate (DMC), methyl ethyl ester (EMC).
In the present invention, described negative material be graphite, carbon, silica-base material, tin-based material one or more.
Beneficial effect of the present invention is: electrolysis additive three (2,2, the 2-trifluoroethyl) borate added contributes to forming stable SEI film in negative terminal surface, stops the common embedding of solvent molecule, suppresses the further reaction of negative pole and electrolyte.Meanwhile, TTFEB adds the composition that can improve SEI film, promotes inert component LiF, Li
2o, Li
2o
2deng, reduce membrane impedance, reduce polarization, reduce the consumption of lithium ion.Due to the improvement result of TTFEB anticathode SEI film, this electrolyte containing TTFEB effectively can improve the cycle performance of negative material, efficiency for charge-discharge and high rate performance.
Accompanying drawing explanation
Fig. 1 adopts the cycle performance of the battery of embodiment 1 and comparative example electrolyte to compare respectively;
Fig. 2 is the cyclic voltammetry curve of the battery adopting embodiment 1 and comparative example electrolyte respectively;
Fig. 3 adopts embodiment 1 and comparative example electrolyte battery high rate performance curve respectively.
Embodiment
Below in conjunction with accompanying drawing, technical scheme of the present invention is further described; but be not limited thereto; everyly technical solution of the present invention modified or equivalent to replace, and not departing from the spirit and scope of technical solution of the present invention, all should be encompassed in protection scope of the present invention.
Embodiment 1:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:DMC=1:2) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 0.5wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 2:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:DMC=3:7) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 0.5wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 3:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:DMC=4:6) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 0.5wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 4:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:EMC=1:2) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 2% fluorinated ethylene carbonate (FEC) and 0.5wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 5:
Ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl ester (EMC) (EC, DMC, EMC mass ratio is EC:DMC:EMC=3:4:3) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 0.5wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 6:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:DMC=1:2) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 1wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 7:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:DMC=1:2) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 2wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 8:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:DMC=4:6) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 1wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Embodiment 9:
Ethylene carbonate (EC), dimethyl carbonate (DMC) and fluorinated ethylene carbonate (FEC) (EC and DMC and FEC mass ratio are EC:DMC:FEC=4:5:1) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, then 1wt% tri-(2 is added, 2,2-trifluoroethyl) borate (TTFEB), described lithium-ion battery electrolytes can be obtained.
Comparative example:
Ethylene carbonate (EC), dimethyl carbonate (DMC) (EC and DMC mass ratio is EC:DMC=1:2) are mixed, to dewater removal of impurities with molecular sieve, 1mol/L lithium hexafluoro phosphate is dissolved in mixed solvent, blank lithium-ion battery electrolytes can be obtained as a comparison.
By the 8:1:1 mixing in mass ratio of graphite, conductive agent acetylene black, binding agent (PVDF), with deionized water, this mixture is modulated into slurry, is evenly coated on Copper Foil, 120 DEG C of vacuumizes, after 12 hours, make experimental cell pole piece.Be to electrode with lithium sheet, electrolyte is the electrolyte prepared in embodiment 1-7 and comparative example, and barrier film is Celgard2400 film, is assembled into graphite/lithium CR2025 type button cell in the glove box being full of argon gas atmosphere.The button cell assembled is carried out charge-discharge performance test: with after the activation of the multiplying power of 0.1C with the circulation 100 times of 1C, voltage range is 0.01-1.5V.Test result is as shown in table 1, and the electrolyte containing additive TTFEB as can be seen from Table 1 can improve the cyclical stability of material.Wherein, Fig. 1 is the cycle performance of battery comparison diagram adopting embodiment 1 and comparative example electrolyte, adopt the cycle performance of the battery of embodiment 1 very stable, after 100 circulations, capacity remains on 346mAh/g, and it is poor to use the cycle performance of battery of comparative example electrolyte to compare, irreversible capacity is comparatively large, and after 100 circulations, capacity drops to 325mAh/g.
On electrochemical workstation, cyclic voltammetry is carried out by adopting the graphite/lithium battery of embodiment 1 and comparative example electrolyte, two curves of comparison diagram 2 can find out that the embedding dealkylation reaction invertibity of the battery lithium ions of circulation in embodiment 1 is higher, polarization reduces, the embedding dealkylation reaction peak of lithium ion becomes large simultaneously, and the embedding de-quantitative change of lithium ion is large.Test shows, TTFEB improves the migration of lithium ion in rete, reduces polarization, improves discharge capacity.
After activating adopting the graphite/lithium battery of embodiment 1 and comparative example electrolyte under the multiplying power of 0.1C, successively with different multiplying: 1C, 2C, 4C, circulate 10 times respectively, Fig. 3 is the high rate performance curve comparison figure of the graphite/lithium battery adopting embodiment 1 and comparative example electrolyte.As seen from the figure, adopt the graphite/lithium battery high rate performance of embodiment 1 electrolyte obviously better than adopting the battery of comparative example electrolyte.When multiplying power becomes after 2C from 1C, adopt the decay of the battery capacity of embodiment 1 electrolyte to only have about 10mAh/g, and use the battery of comparative example electrolyte to have the capacity attenuation of about 34mAh/g.And under 4C multiplying power, use the battery capacity conservation rate of embodiment 1 electrolyte obviously higher, illustrate that TTFEB's adds the high rate performance that obviously can improve graphite.
By the 8:1:1 mixing in mass ratio of nano-silicon negative pole, conductive agent acetylene black, binding agent (SBR+CMC), with deionized water, this mixture is modulated into slurry, is evenly coated on Copper Foil, 120 DEG C of vacuumizes, after 12 hours, make experimental cell pole piece.Be to electrode with lithium sheet, electrolyte is the electrolyte prepared in embodiment 1 and comparative example, is assembled into silicon/lithium CR2025 type button cell in the glove box being full of argon gas atmosphere.The button cell assembled is carried out charge-discharge performance test: with after the activation of the multiplying power of 0.1C with the circulation 30 times of 1C, voltage range is 0.01-1.5V.After 30 circulations, the battery capacity circulated in comparative example electrolyte is only 427mAh/g, and in embodiment 1 electrolyte, cycle battery capacity is increased to 970mAh/g, illustrates that this electrolyte containing TTFEB also improves significantly to silicium cathode SEI film.
Table 1
Claims (5)
1. one kind for improving the electrolyte of lithium ion battery negative material cycle performance, it is characterized in that described electrolyte is made up of organic solvent, lithium salts and additive, wherein: described additive is three (2,2,2-trifluoroethyl) borate, content is in the electrolytic solution 0.1 ~ 5.0wt%; Described organic solvent is made up of cyclic carbonate and linear carbonates, and cyclic carbonate and linear carbonates mass ratio is in the electrolytic solution 1 ~ 5:3 ~ 7; The concentration of described lithium salts is 0.5 ~ 2.5mol/L.
2. the electrolyte for improving lithium ion battery negative material cycle performance according to claim 1, is characterized in that described lithium salts is at least one in lithium hexafluoro phosphate, LiBF4, two trifluoromethanesulfonimide lithium, two (fluorine sulphonyl) imine lithium.
3. the electrolyte for improving lithium ion battery negative material cycle performance according to claim 1, is characterized in that described lithium salts is lithium hexafluoro phosphate.
4. the electrolyte for improving lithium ion battery negative material cycle performance according to claim 1, is characterized in that described cyclic carbonate is one or both in ethylene carbonate or fluorinated ethylene carbonate.
5. the electrolyte for improving lithium ion battery negative material cycle performance according to claim 1, is characterized in that described linear carbonates is at least one or several in diethyl carbonate, dimethyl carbonate, methyl ethyl ester.
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108123172A (en) * | 2016-11-29 | 2018-06-05 | 宁德时代新能源科技股份有限公司 | Electrolyte and secondary lithium battery |
| JP2018106950A (en) * | 2016-12-27 | 2018-07-05 | トヨタ自動車株式会社 | Lithium ion secondary battery |
| CN108539273A (en) * | 2018-04-17 | 2018-09-14 | 广州天赐高新材料股份有限公司 | A kind of novel lithium secondary cell electrolyte and a kind of lithium secondary battery |
| CN109286041A (en) * | 2017-07-19 | 2019-01-29 | 宁德时代新能源科技股份有限公司 | Electrolyte and secondary lithium battery |
| CN110718715A (en) * | 2019-10-23 | 2020-01-21 | 东莞维科电池有限公司 | Battery electrolyte additive, battery electrolyte and lithium ion battery |
| CN112038689A (en) * | 2019-06-04 | 2020-12-04 | 北京卫蓝新能源科技有限公司 | Borate lithium solid electrolyte and application thereof |
| CN112786966A (en) * | 2021-03-01 | 2021-05-11 | 远景动力技术(江苏)有限公司 | Electrolyte and lithium ion battery |
| CN114927759A (en) * | 2022-05-18 | 2022-08-19 | 湖南大学 | Electrolyte with heptafluorobutyryl chloride as additive and lithium ion battery thereof |
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Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108123172A (en) * | 2016-11-29 | 2018-06-05 | 宁德时代新能源科技股份有限公司 | Electrolyte and secondary lithium battery |
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| CN108539273A (en) * | 2018-04-17 | 2018-09-14 | 广州天赐高新材料股份有限公司 | A kind of novel lithium secondary cell electrolyte and a kind of lithium secondary battery |
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| CN110718715A (en) * | 2019-10-23 | 2020-01-21 | 东莞维科电池有限公司 | Battery electrolyte additive, battery electrolyte and lithium ion battery |
| CN110718715B (en) * | 2019-10-23 | 2022-09-27 | 东莞维科电池有限公司 | Battery electrolyte additive, battery electrolyte and lithium ion battery |
| CN112786966A (en) * | 2021-03-01 | 2021-05-11 | 远景动力技术(江苏)有限公司 | Electrolyte and lithium ion battery |
| CN114927759A (en) * | 2022-05-18 | 2022-08-19 | 湖南大学 | Electrolyte with heptafluorobutyryl chloride as additive and lithium ion battery thereof |
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