CN103107363B - Non-water electrolysis solution of lithium ion battery and corresponding lithium ion battery thereof - Google Patents
Non-water electrolysis solution of lithium ion battery and corresponding lithium ion battery thereof Download PDFInfo
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- CN103107363B CN103107363B CN201310038377.1A CN201310038377A CN103107363B CN 103107363 B CN103107363 B CN 103107363B CN 201310038377 A CN201310038377 A CN 201310038377A CN 103107363 B CN103107363 B CN 103107363B
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- Prior art keywords
- lithium ion
- ion battery
- carbonate
- electrolytic solution
- nonaqueous electrolytic
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 43
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 43
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title abstract description 4
- 238000005868 electrolysis reaction Methods 0.000 title abstract 4
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 5
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 5
- 239000003960 organic solvent Substances 0.000 claims abstract description 4
- 239000003792 electrolyte Substances 0.000 claims description 42
- 239000008151 electrolyte solution Substances 0.000 claims description 27
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 26
- OJMIONKXNSYLSR-UHFFFAOYSA-N phosphorous acid Chemical compound OP(O)O OJMIONKXNSYLSR-UHFFFAOYSA-N 0.000 claims description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 15
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical class O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 12
- 229910052799 carbon Inorganic materials 0.000 claims description 12
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 claims description 10
- 239000000463 material Substances 0.000 claims description 10
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 9
- 229910052744 lithium Inorganic materials 0.000 claims description 9
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 7
- 125000000217 alkyl group Chemical group 0.000 claims description 5
- 230000004888 barrier function Effects 0.000 claims description 5
- 150000005676 cyclic carbonates Chemical class 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 4
- 229910013870 LiPF 6 Inorganic materials 0.000 claims description 4
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 4
- 125000001183 hydrocarbyl group Chemical group 0.000 claims description 4
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 3
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 claims description 3
- 229910015015 LiAsF 6 Inorganic materials 0.000 claims description 2
- 229910013063 LiBF 4 Inorganic materials 0.000 claims description 2
- 229910013375 LiC Inorganic materials 0.000 claims description 2
- 229910013528 LiN(SO2 CF3)2 Inorganic materials 0.000 claims description 2
- 229910013385 LiN(SO2C2F5)2 Inorganic materials 0.000 claims description 2
- 229910012513 LiSbF 6 Inorganic materials 0.000 claims description 2
- QBDVHBCBEPBBPL-UHFFFAOYSA-N P(O)(O)O.C(C)(=O)OC=C Chemical compound P(O)(O)O.C(C)(=O)OC=C QBDVHBCBEPBBPL-UHFFFAOYSA-N 0.000 claims description 2
- SIXOAUAWLZKQKX-UHFFFAOYSA-N carbonic acid;prop-1-ene Chemical compound CC=C.OC(O)=O SIXOAUAWLZKQKX-UHFFFAOYSA-N 0.000 claims description 2
- AZEQMGPWGQJEBN-UHFFFAOYSA-N phosphorous acid;prop-1-ene Chemical group CC=C.OP(O)O AZEQMGPWGQJEBN-UHFFFAOYSA-N 0.000 claims description 2
- 125000000383 tetramethylene group Chemical group [H]C([H])([*:1])C([H])([H])C([H])([H])C([H])([H])[*:2] 0.000 claims description 2
- 238000003860 storage Methods 0.000 abstract description 38
- 239000002904 solvent Substances 0.000 abstract description 7
- -1 phosphite ester compound Chemical class 0.000 abstract 2
- 229940125904 compound 1 Drugs 0.000 description 38
- 238000002360 preparation method Methods 0.000 description 27
- 238000012360 testing method Methods 0.000 description 22
- 229910002991 LiNi0.5Co0.2Mn0.3O2 Inorganic materials 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 8
- 239000000654 additive Substances 0.000 description 7
- 229910013716 LiNi Inorganic materials 0.000 description 6
- 229910015645 LiMn Inorganic materials 0.000 description 5
- 230000000996 additive effect Effects 0.000 description 5
- 150000001875 compounds Chemical class 0.000 description 5
- 125000004122 cyclic group Chemical group 0.000 description 5
- 230000014759 maintenance of location Effects 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 3
- 238000000354 decomposition reaction Methods 0.000 description 3
- 229910002804 graphite Inorganic materials 0.000 description 3
- 239000010439 graphite Substances 0.000 description 3
- 238000002347 injection Methods 0.000 description 3
- 239000007924 injection Substances 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 3
- 238000011056 performance test Methods 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- QGHDLJAZIIFENW-UHFFFAOYSA-N 4-[1,1,1,3,3,3-hexafluoro-2-(4-hydroxy-3-prop-2-enylphenyl)propan-2-yl]-2-prop-2-enylphenol Chemical group C1=C(CC=C)C(O)=CC=C1C(C(F)(F)F)(C(F)(F)F)C1=CC=C(O)C(CC=C)=C1 QGHDLJAZIIFENW-UHFFFAOYSA-N 0.000 description 2
- 239000006245 Carbon black Super-P Substances 0.000 description 2
- 229910012820 LiCoO Inorganic materials 0.000 description 2
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 2
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 239000006183 anode active material Substances 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 238000003490 calendering Methods 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 229940125782 compound 2 Drugs 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000012530 fluid Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 2
- 239000010452 phosphate Substances 0.000 description 2
- 150000008301 phosphite esters Chemical class 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 230000004224 protection Effects 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 230000008961 swelling Effects 0.000 description 2
- 229910000314 transition metal oxide Inorganic materials 0.000 description 2
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 102000004310 Ion Channels Human genes 0.000 description 1
- 229910013733 LiCo Inorganic materials 0.000 description 1
- 229910002995 LiNi0.8Co0.15Al0.05O2 Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
- 229910001228 Li[Ni1/3Co1/3Mn1/3]O2 (NCM 111) Inorganic materials 0.000 description 1
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 description 1
- 229910018095 Ni-MH Inorganic materials 0.000 description 1
- 229910018477 Ni—MH Inorganic materials 0.000 description 1
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000005030 aluminium foil Substances 0.000 description 1
- 229910003481 amorphous carbon Inorganic materials 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- MTAZNLWOLGHBHU-UHFFFAOYSA-N butadiene-styrene rubber Chemical compound C=CC=C.C=CC1=CC=CC=C1 MTAZNLWOLGHBHU-UHFFFAOYSA-N 0.000 description 1
- OJIJEKBXJYRIBZ-UHFFFAOYSA-N cadmium nickel Chemical compound [Ni].[Cd] OJIJEKBXJYRIBZ-UHFFFAOYSA-N 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 239000006182 cathode active material Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 229940125898 compound 5 Drugs 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000011258 core-shell material Substances 0.000 description 1
- 238000009831 deintercalation Methods 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910021450 lithium metal oxide Inorganic materials 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 229910001092 metal group alloy Inorganic materials 0.000 description 1
- 239000012982 microporous membrane Substances 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- AICOOMRHRUFYCM-ZRRPKQBOSA-N oxazine, 1 Chemical compound C([C@@H]1[C@H](C(C[C@]2(C)[C@@H]([C@H](C)N(C)C)[C@H](O)C[C@]21C)=O)CC1=CC2)C[C@H]1[C@@]1(C)[C@H]2N=C(C(C)C)OC1 AICOOMRHRUFYCM-ZRRPKQBOSA-N 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 238000004513 sizing Methods 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 125000004417 unsaturated alkyl group Chemical group 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 239000013585 weight reducing agent Substances 0.000 description 1
- 238000003466 welding Methods 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
Classifications
-
- 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
-
- 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
-
- 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
The invention aims to provide a non-water electrolysis solution for a high-performance lithium ion battery. The non-water electrolysis solution comprises a lithium salt, an organic solvent and a phosphite ester compound containing unsaturated bond, wherein the unsaturated phosphite ester compound is contributed to forming a stable compact passivating film (SEI film) on the surface of an electrode, and a solvent molecule is prevented from further decomposing. According to the scheme of the invention, the obtained electrolysis solution can improve a high temperature storage performance and a cycle performance of the battery.
Description
Technical field
The present invention relates to electrochemical field, particularly relate to field of lithium ion secondary.
Background technology
In recent years, portable type electronic product, such as camera, Digital Video, mobile phone, notebook computer etc. are widely used in daily life.Reduce size, weight reduction, increasing the service life is development trend and the requirement of electronic product industry.Therefore, develop the power supply product that matches with portable type electronic product, especially develop and the lightweight secondary cell of high-energy-density can be provided to be the active demand of industry development.
With lead-acid battery, nickel-cadmium cell, Ni-MH battery is compared, and lithium ion battery, because of features such as its energy density is large, operating voltage is high, the life-span is long, environmental protections, is widely used in portable battery product.
Lithium ion battery forms primarily of positive and negative electrode, electrolyte and barrier film.Positive pole is mainly containing the transition metal oxide of lithium, and negative pole is Carbon Materials mainly.Because the average discharge volt of lithium ion battery is about 3.6-3.7V, need electrolyte component stable in the charging/discharging voltages of 0-4.2V.For this reason, lithium ion battery electrolyte used must be nonaqueous electrolytic solution, such as: usually use the mixture comprising cyclic carbonate solvents (as ethylene carbonate) and linear carbonates solvent (as dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate) as solvent, lithium hexafluoro phosphate is as the electrolyte of solute.
Lithium ion battery in initial charge process, lithium ion from the lithium metal oxide of cathode active material deintercalation out, under the driving of voltage anode carbon electrode migration, be then embedded in material with carbon element.In this process, electrolyte and carbon anode surface react, and produce Li
2cO
3, Li
2the materials such as O, LiOH, thus form one deck passivating film at carbon anode surface, this passivating film is referred to as solid electrolyte interface (SEI) film.Owing to no matter being charging or electric discharge, lithium ion must pass through this layer of SEI film, so the performance of SEI film determines many performances (as cycle performance, high-temperature behavior, high rate performance) of battery.SEI film, after initial charge is formed, can stop the further decomposition of electrolyte solvent, and form ion channel in charge and discharge cycles subsequently.But along with the carrying out of discharge and recharge, the expansion that electrode repeats and contraction SEI film may break or dissolve gradually, the anode thereupon exposed continues to react with electrolyte, produce gas simultaneously, thus increase the interior pressure of battery, and significantly reduce the cycle life of battery.Especially battery stores under the high temperature conditions and carries out charge and discharge cycles under the high temperature conditions, and SEI film is more easily destroyed, thus causes battery bulging and cycle performance obviously to decline.The kind of carbonic ester used according to electrolyte and the type of anode active material, the gas of generation mainly comprises CO, CO
2, CH
4, C
2h
6deng.
Due to SEI film quality to the high-temperature storage performance of lithium ion battery and cycle performance most important, the quality therefore improving SEI film by regulation and control is very necessary to realizing high performance lithium ion battery.In order to address this problem, people attempt adding a small amount of additive in the electrolytic solution to improve SEI film, to improving the performance of lithium ion battery.Researcher develops a series of film for additive through great efforts as vinylene carbonate (VC), vinyl ethylene carbonate (VEC), fluorinated ethylene carbonate (FEC) etc., they can form more stable SEI on graphite cathode surface, thus significantly improve the cycle performance of lithium ion battery, also improve high-temperature storage performance to a certain extent, therefore these additives obtain and generally apply in commercial lithium-ion batteries simultaneously.But the SEI that above-mentioned film for additive is formed is still stable not under high-temperature storage conditions, still there will be the decomposition of electrolyte at a higher temperature and cause inflatable, thus bring serious potential safety hazard, be therefore necessary to develop the high-temperature storage performance that new additive improves lithium ion battery further.
Summary of the invention
The object of the invention is to, a kind of high performance lithium ion battery nonaqueous electrolytic solution is provided.
For achieving the above object, the invention provides a kind of lithium ion battery nonaqueous electrolytic solution, comprising:
Lithium salts;
Organic solvent; And
Containing the bi-ester of phosphite of unsaturated bond, this compound is as shown in structural formula 1:
(structural formula 1)
Wherein R
1, R
2, R
3independently be selected from the alkyl that carbon number is 1-4, and R
1, R
2, R
3in at least one is unsaturated alkyl.
Preferably, the described bi-ester of phosphite structure containing unsaturated bond is as shown in structural formula 2:
(structural formula 2)
Wherein R
4be selected from saturated hydrocarbyl or undersaturated alkyl that carbon number is 1-4.
Preferably, the described bi-ester of phosphite structure containing unsaturated bond is as shown in structural formula 3:
(structural formula 3)
Wherein R
5be selected from saturated hydrocarbyl or undersaturated alkyl that carbon number is 1-4.
Preferably, the described bi-ester of phosphite containing unsaturated bond is selected from one of following material or its mixture: tricresyl phosphite vinyl acetate, tricresyl phosphite propylene.
Separately the illustrative compounds in the compound described in structure 1 is illustrated in Table 1, but be not restricted to this.
Table 1
According to lithium ion battery nonaqueous electrolytic solution of the present invention, containing unsaturated bi-ester of phosphite.This unsaturated bi-ester of phosphite contributes to forming stable fine and close passivating film (SEI film) on battery electrode surface, prevents the further decomposition of solvent molecule.High-temperature storage performance and the cycle performance of battery can be improved according to the electrolyte of the solution of the present invention.
According to lithium ion battery nonaqueous electrolytic solution provided by the present invention, be preferably 0.01%-2% by the content in the electrolytic solution of the unsaturated bi-ester of phosphite described in structural formula 1 by electrolyte total weight.Easilier when unsaturated phosphite ester content is in the electrolytic solution not less than 0.01% form effective SEI film on battery electrode surface.It is further preferred that unsaturated phosphite ester can improve the stability of SEI film further when the content of electrolyte is not less than 0.1%, thus improve high-temperature storage performance and the cycle performance of battery further.On the other hand, when unsaturated bi-ester of phosphite content in the electrolytic solution not higher than 2% time, the increase of the internal resistance of cell can be suppressed.It is further preferred that unsaturated bi-ester of phosphite content in the electrolytic solution not higher than 1% time can suppress the increase of the internal resistance of cell further, thus improve high-temperature storage and the cycle performance of battery further.
According to lithium ion battery nonaqueous electrolytic solution provided by the invention, one or more additives in vinylene carbonate (VC), fluorinated ethylene carbonate (FEC), vinyl ethylene carbonate (VEC) can be added further to improve the cycle performance of battery in electrolyte.
Preferably, the solvent of lithium ion battery nonaqueous electrolytic solution of the present invention comprises cyclic carbonate and linear carbonate, cyclic carbonate wherein comprises one or more in ethylene carbonate (EC), propene carbonate (PC), butylene (BC), and linear carbonate wherein comprises one or more in dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (EMC), methyl propyl carbonate (MPC).
The solute of lithium ion battery nonaqueous electrolytic solution of the present invention comprises LiPF
6, LiBF
4, LiSbF
6, LiAsF
6, LiN (SO
2cF
3)
2, LiN (SO
2c
2f
5)
2, LiC (SO
2cF
3)
3, LiN (SO
2f)
2in at least one.Wherein preferably LiPF
6or the mixture of itself and other lithium salts.
Be applied in the lithium ion battery with negative pole and positive pole by lithium ion battery nonaqueous electrolytic solution of the present invention, described negative pole is made up of material with carbon element, metal alloy, lithium-containing oxides and material etc.Wherein, the preferred graphite of material with carbon element or the material with carbon element that is coated on graphite surface with graphite-phase than amorphous carbon and obtains.Described positive electrode preferably adopts lithium-containing transition metal oxide, such as, be selected from one or more in llowing group of materials: LiCoO
2, LiNiO
2, LiMn
2o
4, LiCo
1-ym
yo
2, LiNi
1-ym
yo
2, LiMn
2-ym
yo
4, LiNi
xco
ymn
zm
1-x-y-zo
2, wherein M is selected from one or more in Fe, Co, Ni, Mn, Mg, Cu, Zn, Al, Sn, B, Ga, Cr, Sr, V, Ti, and 0≤y≤1,0≤x≤1,0≤z≤1, x+y+z≤1.
Present invention also offers a kind of lithium ion battery, comprising: lithium ion battery nonaqueous electrolytic solution provided by the invention in foregoing; The positive pole with removal lithium embedded can be embedded; The negative pole with removal lithium embedded can be embedded; And the barrier film be placed between positive pole and negative pole.
In addition present invention also offers above-described unsaturated bi-ester of phosphite and improve the application of aspect of performance of lithium ion battery nonaqueous electrolytic solution and lithium ion battery.
Embodiment
By describing technology contents of the present invention, structural feature in detail, being realized object and effect, be described in detail below in conjunction with execution mode.
Embodiment 1
1) preparation of electrolyte
By ethylene carbonate (EC), diethyl carbonate (DEC) and methyl ethyl carbonate (EMC) in mass ratio for EC:DEC:EMC=1:1:1 mixes, then add lithium hexafluoro phosphate (LiPF
6) to molar concentration be 1mol/L, add the compound 1, the compound 2 that refer in the compound 1(embodiment by the gross mass 0.5% of electrolyte again ... refer to the compound of the reference numeral enumerated in table 1, below each example in like manner) shown in unsaturated bi-ester of phosphite.
2) preparation of positive plate
By the quality of 93:4:3 than blended anode active material lithium nickel cobalt manganese oxide LiNi
0.5co
0.2mn
0.3o
2, then they are dispersed in METHYLPYRROLIDONE (NMP), obtain anode sizing agent by conductive carbon black Super-P and binding agent polyvinylidene fluoride (PVDF).Be uniformly coated on by slurry on the two sides of aluminium foil, through drying, calendering and vacuumize, and burn-on after aluminum lead-out wire with supersonic welder and obtain positive plate, the thickness of pole plate is at 120-150 μm.
3) preparation of negative plate
By the mass ratio mixing negative active core-shell material modified natural graphite of 94:1:2.5:2.5, conductive carbon black Super-P, binding agent butadiene-styrene rubber (SBR) and carboxymethyl cellulose (CMC), then by their dispersions in deionized water, obtain cathode size.Be coated on by slurry on the two sides of Copper Foil, through drying, calendering and vacuumize, and burn-on after nickel making outlet with supersonic welder and obtain negative plate, the thickness of pole plate is at 120-150 μm.
4) preparation of battery core
Between positive plate and negative plate, place thickness is that the polyethene microporous membrane of 20 μm is as barrier film, then the sandwich structure that positive plate, negative plate and barrier film form is reeled, square aluminum metal-back is put into after being flattened by coiling body again, the lead-out wire of both positive and negative polarity is welded on the relevant position of cover plate respectively, and with laser-beam welding machine, cover plate and metal-back are welded as a whole, obtain the battery core treating fluid injection.
5) battery core fluid injection and change into
In the glove box that dew point controls below-40 DEG C, the electrolyte of above-mentioned preparation is injected battery core by liquid injection hole, and the amount of electrolyte will ensure the space be full of in battery core.Then change into according to the following steps: 0.05C constant current charge 3min, 0.2C constant current charge 5min, 0.5C constant current charge 25min, after shelving 1hr, shaping is sealed, then further with the electric current constant current charge of 0.2C to 4.2V, after normal temperature shelf 24hr, with the electric current constant-current discharge of 0.2C to 3.0V.
6) normal-temperature circulating performance test
At room temperature with the electric current constant current charge of 1C to 4.2V then constant voltage charge drop to 0.1C to electric current, then with the electric current constant-current discharge of 1C to 3.0V, circulation like this 300 weeks, records the discharge capacity of the 1st week and the discharge capacity of the 300th week, is calculated as follows the capability retention of normal temperature circulation:
The discharge capacity * 100% of discharge capacity/1st of capability retention=300th week week
7) high temperature cyclic performance test
Battery is placed in the baking oven of constant temperature 45 DEG C, with the electric current constant current charge of 1C to 4.2V then constant voltage charge drop to 0.1C to electric current, then with the electric current constant-current discharge of 1C to 3.0V, circulation like this 300 weeks, record the discharge capacity of the 1st week and the discharge capacity of the 300th week, be calculated as follows the capability retention of high temperature circulation:
The discharge capacity * 100% of discharge capacity/1st of capability retention=300th week week
8) high-temperature storage performance test
At room temperature with the electric current constant current charge of 1C to 4.2V then constant voltage charge drop to 0.1C to electric current, measure the thickness of battery, the baking oven then battery being placed in constant temperature 85 DEG C stores 4h, takes out relief battery cool to room temperature, measure the thickness of battery, be calculated as follows the thickness swelling of battery:
Cell thickness * 100% before thickness swelling=(cell thickness before the cell thickness-storage after storage)/storage
Embodiment 2
Except the compound 2 in the preparation of electrolyte, the compound 1 of 0.5% being changed into 0.5%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 2.
Embodiment 3
Except the compound 5 in the preparation of electrolyte, the compound 1 of 0.5% being changed into 0.5%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 2.
Embodiment 4
Except the compound 7 in the preparation of electrolyte, the compound 1 of 0.5% being changed into 0.5%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 2.
Comparative example 1
Except not adding except compound 1 in the preparation of electrolyte, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 2.
Table 2
As can be seen from the data of table 2, compared with not containing the electrolyte of additive, with the addition of the normal-temperature circulating performance of the battery obtained by electrolyte of unsaturated bi-ester of phosphite, high temperature cyclic performance and high-temperature storage performance and be all significantly improved.
Embodiment 5
Except the compound 1 in the preparation of electrolyte, the compound 1 of 0.5% being changed into 0.01%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 3.
Embodiment 6
Except the compound 1 in the preparation of electrolyte, the compound 1 of 0.5% being changed into 0.1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 3.
Embodiment 7
Except the compound 1 in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 3.
Embodiment 8
Except the compound 1 in the preparation of electrolyte, the compound 1 of 0.5% being changed into 2%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 3.
Table 3
As can be seen from the data of table 3, when compound 1 addition in the electrolytic solution brings up to 0.1% from 0.01%, the normal-temperature circulating performance of battery, high temperature circulation and high-temperature storage performance improve gradually, but when addition is more than 1%, normal-temperature circulating performance and the high temperature cyclic performance of battery decline to some extent, but are still obviously better than the battery not adding compound 1.
Embodiment 9
Except the compound 1 of 0.5% being changed in the preparation of electrolyte into the combination of the vinylene carbonate (VC) of 1% and the compound 1 of 0.5%, other is identical with embodiment 1, tests that the normal temperature obtained circulates, the data of high temperature circulation and high-temperature storage are in table 4.
Embodiment 10
Except the compound 1 of 0.5% being changed in the preparation of electrolyte into the combination of the fluorinated ethylene carbonate (FEC) of 1% and the compound 1 of 0.5%, other is identical with embodiment 1, tests that the normal temperature obtained circulates, the data of high temperature circulation and high-temperature storage are in table 4.
Embodiment 11
Except the compound 1 of 0.5% being changed in the preparation of electrolyte into the combination of the vinyl ethylene carbonate (VEC) of 1% and the compound 1 of 0.5%, other is identical with embodiment 1, tests that the normal temperature obtained circulates, the data of high temperature circulation and high-temperature storage are in table 4.
Comparative example 2
Except the vinylene carbonate (VC) in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 4.
Comparative example 3
Except the fluorinated ethylene carbonate (FEC) in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 4.
Comparative example 4
Except the vinyl ethylene carbonate (VEC) in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 4.
Table 4
As can be seen from the data of table 4, on the basis using VC, FEC or VEC, add compound 1 further and battery can be made to obtain better high-temperature storage performance, normal-temperature circulating performance and high temperature cyclic performance are also improved simultaneously.
Embodiment 12
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiNi into
1/3co
1/3mn
1/3o
2and outside the combination in the preparation of electrolyte, the compound 1 of 0.5% being changed into the vinylene carbonate (VC) of 1% and the compound 1 of 0.5%, other is identical with embodiment 1, tests that the normal temperature obtained circulates, the data of high temperature circulation and high-temperature storage are in table 5.
Embodiment 13
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiNi into
0.8co
0.15al
0.05o
2and outside the combination in the preparation of electrolyte, the compound 1 of 0.5% being changed into the vinylene carbonate (VC) of 1% and the compound 1 of 0.5%, other is identical with embodiment 1, tests that the normal temperature obtained circulates, the data of high temperature circulation and high-temperature storage are in table 5.
Embodiment 14
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiCoO into
2and outside the combination in the preparation of electrolyte, the compound 1 of 0.5% being changed into the vinylene carbonate (VC) of 1% and the compound 1 of 0.5%, other is identical with embodiment 1, tests that the normal temperature obtained circulates, the data of high temperature circulation and high-temperature storage are in table 5.
Embodiment 15
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiMn into
2o
4and outside the combination in the preparation of electrolyte, the compound 1 of 0.5% being changed into the vinylene carbonate (VC) of 1% and the compound 1 of 0.5%, other is identical with embodiment 1, tests that the normal temperature obtained circulates, the data of high temperature circulation and high-temperature storage are in table 5.
Comparative example 5
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiNi into
1/3co
1/3mn
1/3o
2and outside the vinylene carbonate (VC) in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 5.
Comparative example 6
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiNi into
0.8co
0.15al
0.05o
2and outside the vinylene carbonate (VC) in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 5.
Comparative example 7
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiCoO into
2and outside the vinylene carbonate (VC) in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 5.
Comparative example 8
Except by positive electrode LiNi
0.5co
0.2mn
0.3o
2change LiMn into
2o
4and outside the vinylene carbonate (VC) in the preparation of electrolyte, the compound 1 of 0.5% being changed into 1%, other is identical with embodiment 1, test obtain normal temperature circulation, high temperature circulation and high-temperature storage data in table 5.
Table 5
As can be seen from the data of table 5, with LiNi
1/3co
1/3mn
1/3o
2, LiNi
0.8co
0.15al
0.05o
2, LiCoO
2, LiMn
2o
4for in the lithium ion battery of positive electrode, add the high-temperature storage performance that compound 1 also can improve battery, also can improve normal-temperature circulating performance and the high temperature cyclic performance of battery simultaneously.
The foregoing is only embodiments of the invention; not thereby the scope of the claims of the present invention is limited; every utilize description of the present invention to do equivalent structure or equivalent flow process conversion; or be directly or indirectly used in other relevant technical fields, be all in like manner included in scope of patent protection of the present invention.
Claims (8)
1. a lithium ion battery nonaqueous electrolytic solution, comprising:
Lithium salts;
Organic solvent; And
For improving the bi-ester of phosphite containing unsaturated bond of the high-temperature stability of the SEI film that electrode surface is formed,
The described bi-ester of phosphite structure containing unsaturated bond is as shown in structural formula 2 or 3:
Wherein R
4be selected from saturated hydrocarbyl or undersaturated alkyl that carbon number is 1-4;
Wherein R
5be selected from saturated hydrocarbyl or undersaturated alkyl that carbon number is 1-4;
The content of the described bi-ester of phosphite containing unsaturated bond is 0.5% ~ 2% by the total weight of electrolyte.
2. lithium ion battery nonaqueous electrolytic solution according to claim 1, is characterized in that, the described bi-ester of phosphite containing unsaturated bond is selected from one of following material or its mixture: tricresyl phosphite vinyl acetate, tricresyl phosphite propylene.
3. the lithium ion battery nonaqueous electrolytic solution according to claim 1 to 2 any one, it is characterized in that, described lithium ion battery nonaqueous electrolytic solution is also containing one or more in following material: vinylene carbonate, fluorinated ethylene carbonate, vinyl ethylene carbonate.
4. the lithium ion battery nonaqueous electrolytic solution according to claim 1 to 2 any one, is characterized in that, described organic solvent is the mixture of cyclic carbonate and linear carbonate.
5. lithium ion battery nonaqueous electrolytic solution according to claim 4, is characterized in that, described cyclic carbonate comprises: one or more in ethylene carbonate, propene carbonate, butylene.
6. lithium ion battery nonaqueous electrolytic solution according to claim 4, is characterized in that, described linear carbonate comprises: one or more in dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate.
7. the lithium ion battery nonaqueous electrolytic solution according to claim 1 to 2 any one, is characterized in that, described lithium salts is selected from: LiPF
6, LiBF
4, LiSbF
6, LiAsF
6, LiN (SO
2cF
3)
2, LiN (SO
2c
2f
5)
2, LiC (SO
2cF
3)
3, LiN (SO
2f)
2in at least one.
8. a lithium ion battery, comprising:
Lithium ion battery nonaqueous electrolytic solution described in claim 1 to 7 any one;
The positive pole with removal lithium embedded can be embedded;
The negative pole with removal lithium embedded can be embedded; And
Be placed in the barrier film between positive pole and negative pole.
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| PCT/CN2013/072310 WO2014117421A1 (en) | 2013-01-31 | 2013-03-07 | Non-aqueous electrolyte for lithium ion batteries and corresponding lithium ion battery thereof |
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| WO2015015883A1 (en) * | 2013-07-31 | 2015-02-05 | 日本電気株式会社 | Lithium secondary battery and electrolyte solution for lithium secondary batteries |
| CN103880881B (en) * | 2014-04-16 | 2016-05-18 | 苏州科技学院相城研究院 | A kind of preparation method of Dimethyl ally phosphite |
| CN105140561A (en) * | 2015-07-08 | 2015-12-09 | 深圳新宙邦科技股份有限公司 | Non-aqueous electrolyte of lithium ion battery and lithium ion battery |
| CN105336987A (en) * | 2015-11-17 | 2016-02-17 | 深圳新宙邦科技股份有限公司 | Non-aqueous electrolyte of lithium ion battery and lithium ion battery |
| CN107516745B (en) * | 2017-08-16 | 2019-09-03 | 中节能万润股份有限公司 | A kind of non-aqueous electrolyte for lithium ion cell |
| CN108649265A (en) * | 2018-05-10 | 2018-10-12 | 桑德集团有限公司 | Electrolysis additive, lithium battery electrolytes and lithium battery |
| US11961967B2 (en) | 2018-10-30 | 2024-04-16 | Enevate Corporation | Silicon-based energy storage devices with phosphorus containing electrolyte additives |
| CN111384438B (en) * | 2018-12-29 | 2022-10-18 | 深圳新宙邦科技股份有限公司 | Lithium ion battery non-aqueous electrolyte and lithium ion battery |
| WO2020135668A1 (en) * | 2018-12-29 | 2020-07-02 | 深圳新宙邦科技股份有限公司 | Non-aqueous electrolyte for lithium-ion battery, and lithium-ion battery |
| CN111384391B (en) * | 2018-12-29 | 2022-03-11 | 深圳新宙邦科技股份有限公司 | High-nickel lithium ion battery |
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| JP4910239B2 (en) * | 2000-12-25 | 2012-04-04 | 三菱化学株式会社 | Non-aqueous electrolyte secondary battery |
| JP4236390B2 (en) * | 2001-04-19 | 2009-03-11 | 三洋電機株式会社 | Lithium secondary battery |
| JP2004014351A (en) * | 2002-06-07 | 2004-01-15 | Matsushita Electric Ind Co Ltd | Nonaqueous electrolyte secondary battery |
| US7638243B2 (en) * | 2006-03-22 | 2009-12-29 | Novolyte Technologies Inc. | Stabilized nonaqueous electrolytes for rechargeable batteries |
| CN101079505B (en) * | 2007-05-11 | 2010-05-26 | 武汉大学 | Combustion-resisting electrolyte of lithium secondary cell and its lithium cell |
| CN101383433B (en) * | 2008-10-17 | 2010-12-22 | 汕头市金光高科有限公司 | Stabilizer for non-water electrolysis and non-water electrolysis containing the stabilizer |
| CN101914259B (en) * | 2010-08-11 | 2012-02-01 | 华南理工大学 | Material special for preparing lithium ion battery diaphragm and preparation method thereof |
| CN102386441A (en) * | 2011-10-21 | 2012-03-21 | 厦门大学 | Double-functional lithium battery electrolyte additive and preparation method thereof |
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