CN105206874A - Alkynyl silane containing lithium-ion battery electrolyte and lithium-ion battery utilizing same - Google Patents
Alkynyl silane containing lithium-ion battery electrolyte and lithium-ion battery utilizing same Download PDFInfo
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- CN105206874A CN105206874A CN201510681106.7A CN201510681106A CN105206874A CN 105206874 A CN105206874 A CN 105206874A CN 201510681106 A CN201510681106 A CN 201510681106A CN 105206874 A CN105206874 A CN 105206874A
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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
- H01M10/056—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
- H01M10/0569—Liquid materials characterised by the solvents
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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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- Condensed Matter Physics & Semiconductors (AREA)
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Abstract
The invention discloses an alkynyl silane containing lithium-ion battery electrolyte and a lithium-ion battery utilizing the same. The electrolyte comprises electrolyte lithium salt, non-water organic solvents and an additive, wherein the additive comprises at leaset one alkynyl silane compound shown in the structural formula I in the specification, wherein each of R1, R2 and R3 in the formula I represents any one of an alkyl group with the carbon atom number ranging from 1 to 3 and fluoroalkyl separately, and Y represents any one of a hydrogen atom, a component shown in the specification, a phenyl group and a component shown in the specification. The alkynyl silane molecular structure contains a carbon-carbon triple bond functional group and can react on the surface of an electrode preferably to form a good electrode interface protection film, and the formed silicon-containing protection film is good in stability and low in charge transfer resistance. The cycle performance of the lithium ion battery utilizing the electrolyte is excellent under the high voltage being 4.35V and has the characteristics of little gas produced during storage at high temperature and high low-temperature discharge proportion.
Description
Technical field
The present invention relates to field of lithium ion battery, be specifically related to a kind of lithium-ion battery electrolytes containing alkynyl silane and use the lithium ion battery of this electrolyte.
Background technology
Lithium ion battery has that operating voltage is high, specific capacity is large, have extended cycle life, memory-less effect and the advantage such as environmentally friendly, is widely used in the fields such as number, energy storage, power and militay space flight aviation.
Electrolyte is the important component part of lithium ion battery, as the carrier of lithium ion battery intermediate ion transmission, plays vital effect to the performance of lithium ion battery various aspects of performance.Along with the fast development in terminal applies field, the requirement of lithium ion battery not only demand fulfillment more high-energy-density, need to take into account high temperature performance, this has higher requirement to electrolyte property simultaneously.
Current lithium-ion battery electrolytes adopts cyclic carbonate and linear carbonate as mixed organic solvents substantially.By the impact of the multiple factors such as mixed organic solvents liquid journey scope, SEI film thermal stability and the impedance of SEI membrane interface, lithium ion battery is difficult to effectively take into account high temperature performance, particularly for the real battery system of high voltage, seems particularly outstanding.
Summary of the invention
The present invention is directed to above background technology, provide a kind of and contain the lithium-ion battery electrolytes of alkynyl silane and use the lithium ion battery of this electrolyte, to improve cycle performance and the high temperature performance of the real battery system of high voltage.
To achieve these goals, the present invention is achieved through the following technical solutions:
A lithium-ion battery electrolytes containing alkynyl silane, it is characterized in that, described electrolyte is made up of electrolyte lithium salt, non-aqueous organic solvent and additive, comprises the alkynyl silane compound of at least one as shown in structural formula I in additive:
(structural formula I), R in formula I
1, R
2, R
3represent that carbon number is alkyl and any one of fluoro-alkyl of 1 ~ 3 independently of one another, Y be hydrogen atom,
phenyl and
any one.
R in described structural formula I
1, R
2, R
3be methyl.
Alkynyl silane compound shown in described structural formula I is trimethyl silicane ethyl-acetylene, two (trimethyl silyl) acetylene, phenylacetylene base trimethyl silane or Isosorbide-5-Nitrae-bis-(TMS)-1,3-diacetylene.
Alkynyl silane compound amount shown in described structural formula I accounts for 0.5 ~ 5.0% of electrolyte gross mass.
Described electrolyte lithium salt is LiPF
6, LiBOB, LiDFOB, LiBF
4, at least one in LiTFSI, LiFSI.
Described non-aqueous organic solvent be in ethylene carbonate, propene carbonate, methyl ethyl carbonate, dimethyl carbonate, diethyl carbonate, methyl propyl carbonate two or more.
Described additive also comprise in vinylene carbonate, 1,3-propane sultone, sulfuric acid vinyl ester, methane-disulfonic acid methylene ester, fluorinated ethylene carbonate, adiponitrile, 1,2-bis-(2-cyanoethoxyl) ethane any one and more than; It accounts for 0.5% ~ 10.0% of lithium-ion battery electrolytes gross mass.
A kind of lithium ion battery: comprise positive plate, negative plate, barrier film and the lithium-ion battery electrolytes containing alkynyl silane described above; Described positive plate active material be cobalt acid lithium, nickle cobalt lithium manganate or nickel cobalt lithium aluminate in any one, described negative plate active material be in graphite, Si-C composite material any one.
The invention has the advantages that:
Containing carbon carbon triple bond functionality in the alkynyl silane molecular structure that the present invention is used, preferentially can react at electrode surface, form good electrode interface diaphragm, the siliceous diaphragm Heat stability is good formed, charge transfer impedance are low.Use the lithium ion battery of this electrolyte being greater than cycle performance excellence under 4.35V high voltage, there is the feature that high-temperature storage aerogenesis is few and low temperature discharge ratio is high simultaneously.
Embodiment
Below by exemplary embodiment, the present invention will be further elaborated; But scope of the present invention should not be limited to the scope of embodiment, any do not depart from purport of the present invention change or change and can be understood by those skilled in the art, all within protection scope of the present invention.
Embodiment 1
In the glove box being full of argon gas, 1:1:1 takes ethylene carbonate respectively in mass ratio, diethyl carbonate, methyl ethyl carbonate be made into mixed solvent, then in mixed solvent, the additive of following electrolyte quality ratio is added successively: 2.0wt% two (trimethyl silyl) acetylene, 3.0wt% fluorinated ethylene carbonate, 1.0wt% sulfuric acid vinyl ester, slowly add in the most backward mixed liquor and account for electrolyte quality than the LiPF for 12.0wt%
6, after stirring, obtain the lithium-ion battery electrolytes of embodiment 1.
Embodiment 2
In the glove box being full of argon gas, 3:5:2 takes ethylene carbonate respectively in mass ratio, diethyl carbonate, methyl ethyl carbonate be made into mixed solvent, then in mixed solvent, add the additive of following electrolyte quality ratio successively: 1.0wt% phenylacetylene base trimethyl silane, 2.0wt% fluorinated ethylene carbonate, 2.0wt% adiponitrile, 1.0wt%LiBOB, slowly add in the most backward mixed liquor and account for electrolyte quality than the LiPF for 12.0wt%
6, after stirring, obtain the lithium-ion battery electrolytes of embodiment 2.
Embodiment 3
In the glove box being full of argon gas, 3:6:1 takes ethylene carbonate respectively in mass ratio, diethyl carbonate, propene carbonate be made into mixed solvent, then in mixed solvent, the additive of following electrolyte quality ratio is added successively: 1wt%1, two (TMS)-1 of 4-, 3-diacetylene, 3.0wt% fluorinated ethylene carbonate, 1.0wt%1,2-bis-(2-cyanoethoxyl) ethane, 2.0wt%1,3-propane sultone, slowly adds in the most backward mixed liquor and accounts for electrolyte quality than the LiPF for 13.0wt%
6, after stirring, obtain the lithium-ion battery electrolytes of embodiment 3.
Comparative example 1
In the glove box being full of argon gas, 1:1:1 takes ethylene carbonate respectively in mass ratio, diethyl carbonate, methyl ethyl carbonate be made into mixed solvent, then in mixed solvent, add the additive of following electrolyte quality ratio successively: 3.0wt% fluorinated ethylene carbonate, 1.0wt% sulfuric acid vinyl ester, slowly add in the most backward mixed liquor and account for electrolyte quality than the LiPF for 12.0wt%
6, after stirring, obtain the lithium-ion battery electrolytes of comparative example 1.
Comparative example 2
In the glove box being full of argon gas, 3:5:2 takes ethylene carbonate respectively in mass ratio, diethyl carbonate, methyl ethyl carbonate be made into mixed solvent, then in mixed solvent, add the additive of following electrolyte quality ratio successively: 2.0wt% fluorinated ethylene carbonate, 2.0wt% adiponitrile, 1.0wt%LiBOB, slowly add in the most backward mixed liquor and account for electrolyte quality than the LiPF for 12.0wt%
6, after stirring, obtain the lithium-ion battery electrolytes of comparative example 2.
Comparative example 3
In the glove box being full of argon gas, 3:6:1 takes ethylene carbonate respectively in mass ratio, diethyl carbonate, propene carbonate be made into mixed solvent, then in mixed solvent, the additive of following electrolyte quality ratio is added successively: 3.0wt% fluorinated ethylene carbonate, 1.0wt%1,2-bis-(2-cyanoethoxyl) ethane, 2.0wt%1,3-propane sultone, slowly adds in the most backward mixed liquor and accounts for electrolyte quality than the LiPF for 13.0wt%
6, after stirring, obtain the lithium-ion battery electrolytes of comparative example 3.
Lithium-ion battery electrolytes prepared by the lithium-ion battery electrolytes prepare above-described embodiment 1 ~ 3 and comparative example 1 ~ 3 injects through fully dry graphite/LiCoO
2battery, battery leaves standstill through an envelope, change into, carry out 3.0V ~ 4.35V1C cycle charge discharge electrical testing after two envelope partial volumes, the full electric state 85 DEG C/6H of 4.35V stores test and the test of-20 DEG C/0.2C low temperature discharge.
3.0V ~ 4.35V1C cycle charge discharge electrical testing:
Under the condition of room temperature 25 ± 2 DEG C, carry out the test of 3.0V-4.35V circulating battery to embodiment and comparative example experimental cell, testing procedure is: A, 1C constant current charge is to 4.35V, and then constant voltage charge is to cut-off current 0.01C, leaves standstill 5 minutes; B, 1C constant-current discharge, to 3.0V, leaves standstill 5 minutes; C, circulation step A and B, cycle-index is 300 times.300 cycle capability retention=300 cycle capacity/battery capacity * 100% first.
Test result is as shown in table 1:
| Test index | Battery is capacity/mAh first | 300 cycle capacity/mAh | 300 cycle capability retentions |
| Embodiment 1 | 1530 | 1347 | 88.0 |
| Embodiment 2 | 1521 | 1345 | 88.4 |
| Embodiment 3 | 1532 | 1356 | 88.5 |
| Comparative example 1 | 1515 | 1232 | 81.3 |
| Comparative example 2 | 1510 | 1233 | 81.7 |
| Comparative example 3 | 1514 | 1248 | 82.4 |
Table 1
The full electric state 85 DEG C/6H of 4.35V stores test:
A, embodiment and comparative example experimental cell are carried out to the 0.5C charge-discharge test of 3.0V-4.35V voltage range under the condition of room temperature 25 ± 2 DEG C, capacity before record stores; B, 0.5C constant-current constant-voltage charging is to 4.35V, and cut-off current is 0.01C, the full electric state thickness of test battery; C, full electric state battery is transferred in 85 DEG C of insulating boxs, stores the hot thickness of test battery after 6 hours, thickness * 100% before hot thickness swelling=(before the hot thickness-storage of battery thickness)/store; D, by cooled battery 0.5C constant-current discharge to 3.0V, residual capacity after record stores, the front capacity * 100% of residual capacity/storage after battery capacity surplus ratio=storages; E, battery is carried out 0.5C charge-discharge test again, record can recover capacity after storing, and can recover the front capacity * 100% of capacity/storages after capacity resuming rate=storage.Test result is as shown in table 2:
-20 DEG C/0.2C low temperature discharge is tested:
A, under the condition of room temperature 25 ± 2 DEG C to embodiment and comparative example experimental cell carry out 3.0V-4.35V voltage range 1C constant-current constant-voltage charging, 0.2C constant-current discharge test, record 25 ± 2 DEG C of battery 0.2C discharge capacities; B, 1C constant-current constant-voltage charging is to 4.35V, and cut-off current is 0.01C; C, full electric state battery is transferred in-20 DEG C of insulating boxs, constant temperature is shelved after 6 hours and is carried out 0.2C constant-current discharge to 3.0V, record-20 DEG C of battery 0.2C discharge capacities, D, DEG C battery 0.2C discharge capacity/25 ± 2 ,-20 DEG C/0.2C low temperature discharge ratio=-20 DEG C battery 0.2C discharge capacity * 100%.Test result is as shown in table 2:
Table 2 embodiment and comparative example battery high temperature performance test result
From table 1 and table 2 result: add any one alkynyl silane compound in the present invention shown in structural formula I in electrolyte, effectively can promote lithium ion battery and be greater than the combination property under 4.35V operating high voltage.Use lithium ion battery prepared by electrolyte provided by the invention, not only cycle performance is excellent, has the feature that high-temperature storage aerogenesis is few and low temperature discharge ratio is high simultaneously.
The foregoing is only embodiments of the invention, not thereby limit the scope of the claims of the present invention, every equivalence utilizing description of the present invention to do is replaced, and all should be included in scope of patent protection of the present invention.
Claims (8)
1. the lithium-ion battery electrolytes containing alkynyl silane, it is characterized in that, described electrolyte is made up of electrolyte lithium salt, non-aqueous organic solvent and additive, comprises the alkynyl silane compound of at least one as shown in structural formula I in additive:
(structural formula I), R in formula I
1, R
2, R
3represent that carbon number is alkyl and any one of fluoro-alkyl of 1 ~ 3 independently of one another, Y represent hydrogen atom,
phenyl and
any one.
2. the lithium-ion battery electrolytes containing alkynyl silane according to claim 1, is characterized in that, the R in described structural formula I
1, R
2, R
3be methyl.
3. the lithium-ion battery electrolytes containing alkynyl silane according to claim 1, it is characterized in that, alkynyl silane compound shown in described structural formula I is trimethyl silicane ethyl-acetylene, two (trimethyl silyl) acetylene, phenylacetylene base trimethyl silane or 1,4-two (TMS)-1,3-diacetylene.
4. the lithium-ion battery electrolytes containing alkynyl silane according to claim 1, it is characterized in that, the alkynyl silane compound amount shown in described structural formula I accounts for 0.5 ~ 5.0% of electrolyte gross mass.
5. the lithium-ion battery electrolytes containing alkynyl silane according to claim 1, it is characterized in that, described electrolyte lithium salt is LiPF
6, LiBOB, LiDFOB, LiBF
4, at least one in LiTFSI, LiFSI.
6. the lithium-ion battery electrolytes containing alkynyl silane according to claim 1, it is characterized in that, described non-aqueous organic solvent be in ethylene carbonate, propene carbonate, methyl ethyl carbonate, dimethyl carbonate, diethyl carbonate, methyl propyl carbonate two or more.
7. the lithium-ion battery electrolytes containing alkynyl silane according to claim 1, it is characterized in that, described additive also comprises vinylene carbonate, 1, in 3-propane sultone, sulfuric acid vinyl ester, methane-disulfonic acid methylene ester, fluorinated ethylene carbonate, adiponitrile, 1,2-bis-(2-cyanoethoxyl) ethane any one and more than; It accounts for 0.5% ~ 10.0% of lithium-ion battery electrolytes gross mass.
8. a lithium ion battery: comprise the lithium-ion battery electrolytes containing alkynyl silane described in positive plate, negative plate, barrier film and claim 1-7 any one; Described positive plate active material be cobalt acid lithium, nickle cobalt lithium manganate or nickel cobalt lithium aluminate in any one, described negative plate active material be in graphite, Si-C composite material any one.
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| CN105789686A (en) * | 2016-03-18 | 2016-07-20 | 东莞市凯欣电池材料有限公司 | High-capacity lithium ion battery electrolyte and high-capacity lithium ion battery |
| EP3416229A4 (en) * | 2016-02-08 | 2019-03-20 | Central Glass Co., Ltd. | Electrolytic solution for nonaqueous electrolytic solution battery, and nonaqueous electrolytic solution battery using same |
| CN110416614A (en) * | 2019-08-02 | 2019-11-05 | 湖州昆仑动力电池材料有限公司 | A kind of nickelic electrolyte for lithium ion battery |
| CN111029650A (en) * | 2017-02-13 | 2020-04-17 | 宁德新能源科技有限公司 | Electrolyte and secondary battery |
| CN111211355A (en) * | 2020-01-15 | 2020-05-29 | 松山湖材料实验室 | High-voltage lithium ion battery electrolyte additive, electrolyte and battery thereof |
| CN111416154A (en) * | 2020-05-22 | 2020-07-14 | 松山湖材料实验室 | Silicon-based pyridine additive for high-voltage lithium ion battery electrolyte, electrolyte and battery |
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| CN112467208A (en) * | 2019-09-09 | 2021-03-09 | 珠海冠宇电池股份有限公司 | Silicon-carbon lithium ion battery containing non-aqueous electrolyte and preparation method and application thereof |
| CN112467205A (en) * | 2019-09-09 | 2021-03-09 | 珠海冠宇电池股份有限公司 | High-voltage non-aqueous electrolyte and lithium ion battery containing same |
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| CN114069045A (en) * | 2020-07-31 | 2022-02-18 | 浙江中蓝新能源材料有限公司 | Silane additive composition, electrolyte containing same and lithium ion battery |
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| CN110416614B (en) * | 2019-08-02 | 2022-08-26 | 湖州昆仑亿恩科电池材料有限公司 | Electrolyte for high-nickel lithium ion battery |
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