CN112713308A - Non-aqueous electrolyte and lithium ion battery based on same - Google Patents
Non-aqueous electrolyte and lithium ion battery based on same Download PDFInfo
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- CN112713308A CN112713308A CN202011606959.1A CN202011606959A CN112713308A CN 112713308 A CN112713308 A CN 112713308A CN 202011606959 A CN202011606959 A CN 202011606959A CN 112713308 A CN112713308 A CN 112713308A
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- Prior art keywords
- lithium
- carbonate
- electrolyte
- oxalato
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 26
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 26
- 239000011255 nonaqueous electrolyte Substances 0.000 title abstract description 7
- 239000003792 electrolyte Substances 0.000 claims abstract description 68
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 48
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 31
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims abstract description 18
- 229910019142 PO4 Inorganic materials 0.000 claims abstract description 18
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims abstract description 18
- 239000010452 phosphate Substances 0.000 claims abstract description 18
- 239000000654 additive Substances 0.000 claims abstract description 15
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 12
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 12
- 239000002904 solvent Substances 0.000 claims description 19
- 239000011356 non-aqueous organic solvent Substances 0.000 claims description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 12
- 239000008151 electrolyte solution Substances 0.000 claims description 11
- 230000000996 additive effect Effects 0.000 claims description 9
- -1 lithium hexafluorophosphate Chemical compound 0.000 claims description 9
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 6
- 239000000463 material Substances 0.000 claims description 6
- 150000004649 carbonic acid derivatives Chemical class 0.000 claims description 5
- 239000006258 conductive agent Substances 0.000 claims description 5
- 150000005676 cyclic carbonates Chemical class 0.000 claims description 5
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 5
- 239000007773 negative electrode material Substances 0.000 claims description 5
- 239000007774 positive electrode material Substances 0.000 claims description 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 4
- 239000006230 acetylene black Substances 0.000 claims description 4
- 150000001733 carboxylic acid esters Chemical class 0.000 claims description 4
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 4
- ZPFAVCIQZKRBGF-UHFFFAOYSA-N 1,3,2-dioxathiolane 2,2-dioxide Chemical compound O=S1(=O)OCCO1 ZPFAVCIQZKRBGF-UHFFFAOYSA-N 0.000 claims description 3
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 3
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 3
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 3
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 claims description 3
- DSMUTQTWFHVVGQ-UHFFFAOYSA-N 4,5-difluoro-1,3-dioxolan-2-one Chemical compound FC1OC(=O)OC1F DSMUTQTWFHVVGQ-UHFFFAOYSA-N 0.000 claims description 2
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 2
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 2
- 229910016133 LiNi1-x-y-zCoxMnyAlzO2 Inorganic materials 0.000 claims description 2
- RJUFJBKOKNCXHH-UHFFFAOYSA-N Methyl propionate Chemical compound CCC(=O)OC RJUFJBKOKNCXHH-UHFFFAOYSA-N 0.000 claims description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 2
- OBNDGIHQAIXEAO-UHFFFAOYSA-N [O].[Si] Chemical compound [O].[Si] OBNDGIHQAIXEAO-UHFFFAOYSA-N 0.000 claims description 2
- 229910045601 alloy Inorganic materials 0.000 claims description 2
- 239000000956 alloy Substances 0.000 claims description 2
- 229910021383 artificial graphite Inorganic materials 0.000 claims description 2
- 239000011230 binding agent Substances 0.000 claims description 2
- WLLOZRDOFANZMZ-UHFFFAOYSA-N bis(2,2,2-trifluoroethyl) carbonate Chemical compound FC(F)(F)COC(=O)OCC(F)(F)F WLLOZRDOFANZMZ-UHFFFAOYSA-N 0.000 claims description 2
- 239000004917 carbon fiber Substances 0.000 claims description 2
- 239000002041 carbon nanotube Substances 0.000 claims description 2
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 2
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 claims description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 2
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 2
- 239000003273 ketjen black Substances 0.000 claims description 2
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 2
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 claims description 2
- GBPVMEKUJUKTBA-UHFFFAOYSA-N methyl 2,2,2-trifluoroethyl carbonate Chemical compound COC(=O)OCC(F)(F)F GBPVMEKUJUKTBA-UHFFFAOYSA-N 0.000 claims description 2
- 229940017219 methyl propionate Drugs 0.000 claims description 2
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 2
- 229910021382 natural graphite Inorganic materials 0.000 claims description 2
- 229940090181 propyl acetate Drugs 0.000 claims description 2
- HUAZGNHGCJGYNP-UHFFFAOYSA-N propyl butyrate Chemical compound CCCOC(=O)CCC HUAZGNHGCJGYNP-UHFFFAOYSA-N 0.000 claims description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 2
- 229910052710 silicon Inorganic materials 0.000 claims description 2
- 239000010703 silicon Substances 0.000 claims description 2
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 claims description 2
- LSGOVYNHVSXFFJ-UHFFFAOYSA-N vanadate(3-) Chemical compound [O-][V]([O-])([O-])=O LSGOVYNHVSXFFJ-UHFFFAOYSA-N 0.000 claims description 2
- 239000003660 carbonate based solvent Substances 0.000 claims 4
- KLARSDUHONHPRF-UHFFFAOYSA-N [Li].[Mn] Chemical compound [Li].[Mn] KLARSDUHONHPRF-UHFFFAOYSA-N 0.000 claims 1
- 150000001732 carboxylic acid derivatives Chemical class 0.000 claims 1
- OVAQODDUFGFVPR-UHFFFAOYSA-N lithium cobalt(2+) dioxido(dioxo)manganese Chemical compound [Li+].[Mn](=O)(=O)([O-])[O-].[Co+2] OVAQODDUFGFVPR-UHFFFAOYSA-N 0.000 claims 1
- BDKWOJYFHXPPPT-UHFFFAOYSA-N lithium dioxido(dioxo)manganese nickel(2+) Chemical compound [Mn](=O)(=O)([O-])[O-].[Ni+2].[Li+] BDKWOJYFHXPPPT-UHFFFAOYSA-N 0.000 claims 1
- 239000012528 membrane Substances 0.000 abstract description 16
- 238000002156 mixing Methods 0.000 description 20
- 229910012258 LiPO Inorganic materials 0.000 description 11
- 238000002360 preparation method Methods 0.000 description 11
- 229910001290 LiPF6 Inorganic materials 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 10
- 229910013188 LiBOB Inorganic materials 0.000 description 9
- 239000000203 mixture Substances 0.000 description 6
- 239000002033 PVDF binder Substances 0.000 description 4
- 239000004698 Polyethylene Substances 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- 229920000573 polyethylene Polymers 0.000 description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 4
- 229910013075 LiBF Inorganic materials 0.000 description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 3
- 238000005056 compaction Methods 0.000 description 3
- 238000002347 injection Methods 0.000 description 3
- 239000007924 injection Substances 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 2
- 229910013872 LiPF Inorganic materials 0.000 description 2
- 101150058243 Lipf gene Proteins 0.000 description 2
- MYRUXGCOHIYOBX-UHFFFAOYSA-K [Li+].[Li+].[Li+].[O-]P([O-])([O-])=O.FOC(=O)C(=O)OF Chemical compound [Li+].[Li+].[Li+].[O-]P([O-])([O-])=O.FOC(=O)C(=O)OF MYRUXGCOHIYOBX-UHFFFAOYSA-K 0.000 description 2
- 239000000853 adhesive Substances 0.000 description 2
- 230000001070 adhesive effect Effects 0.000 description 2
- 230000032683 aging Effects 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- 239000001768 carboxy methyl cellulose Substances 0.000 description 2
- 239000010406 cathode material Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000004806 packaging method and process Methods 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 238000002791 soaking Methods 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
- 229910013716 LiNi Inorganic materials 0.000 description 1
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000011247 coating layer Substances 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 238000007731 hot pressing Methods 0.000 description 1
- 239000012943 hotmelt Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- DEUISMFZZMAAOJ-UHFFFAOYSA-N lithium dihydrogen borate oxalic acid Chemical compound B([O-])(O)O.C(C(=O)O)(=O)O.C(C(=O)O)(=O)O.[Li+] DEUISMFZZMAAOJ-UHFFFAOYSA-N 0.000 description 1
- FRMOHNDAXZZWQI-UHFFFAOYSA-N lithium manganese(2+) nickel(2+) oxygen(2-) Chemical compound [O-2].[Mn+2].[Ni+2].[Li+] FRMOHNDAXZZWQI-UHFFFAOYSA-N 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 230000003446 memory effect Effects 0.000 description 1
- HNQIVZYLYMDVSB-UHFFFAOYSA-N methanesulfonimidic acid Chemical compound CS(N)(=O)=O HNQIVZYLYMDVSB-UHFFFAOYSA-N 0.000 description 1
- WKFBZNUBXWCCHG-UHFFFAOYSA-N phosphorus trifluoride Chemical compound FP(F)F WKFBZNUBXWCCHG-UHFFFAOYSA-N 0.000 description 1
- 239000002985 plastic film Substances 0.000 description 1
- 229920006255 plastic film Polymers 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 150000005685 straight-chain carbonates Chemical class 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 238000003466 welding Methods 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
- H01M10/056—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
-
- 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
-
- 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
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Secondary Cells (AREA)
Abstract
The invention relates to a non-aqueous electrolyte and a lithium ion battery based on the same, wherein lithium salt additives, namely lithium bis (oxalato) borate and lithium difluoro (oxalato) phosphate are added, and the lithium bis (oxalato) borate and the lithium difluoro (oxalato) phosphate are matched with central atoms of the lithium bis (oxalato) borate and the lithium difluoro (oxalato) phosphate to be re-bonded with electrolyte membranes with similar groups around, so that the electrolyte membranes are prevented from continuously growing, stable P, B end groups are formed, the thickness and the stability of electrode surface membranes are controlled, and the performances of low impedance increase and long circulation at different temperatures are realized.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a non-aqueous electrolyte and a lithium ion battery based on the same.
Background
The lithium ion battery has the advantages of high specific energy, no memory effect, long cycle life and the like, so that the lithium ion battery is generally applied to the field of 3C consumer electronics products such as mobile phones and notebook computers, and in addition, along with the rapid development of new energy automobiles, the application of the lithium ion battery in the fields of power and energy storage is more and more common. With the increase of the endurance mileage of the electric vehicle and the gradual decrease of national subsidies, the requirement on the energy density of the power battery is higher and higher, and at present, the effective methods are to improve the voltage and the compaction density of the electrode active material and select a proper electrolyte.
In order to increase the capacity of the battery, the use of a high-voltage cathode material is an effective way to increase the capacity density of the lithium ion battery, and at high voltage, the electrolyte is easily decomposed, the additive is gradually reduced, the internal resistance of the battery is increased and a large amount of heat is generated along with the continuous charging of the battery, and the cycle life is generally deteriorated after many charging and discharging cycles.
Therefore, it is particularly important to develop more and more novel electrolytes matched with high-voltage cathode materials.
Disclosure of Invention
In order to solve the technical problems, the invention aims to provide a non-aqueous electrolyte, lithium salt additives, namely lithium bis (oxalato) borate and lithium difluoro (oxalato) phosphate are added, central atoms of the lithium bis (oxalato) borate and the lithium difluoro (oxalato) phosphate are matched with each other, and the lithium bis (oxalato) borate and the lithium difluoro (oxalato) phosphate are re-bonded with electrolyte membranes with similar groups around, so that the electrolyte membranes are prevented from continuously growing, stable P, B terminal groups are formed, the thickness and the stability of electrode surface membranes are controlled, and the performance of low impedance increase and long cycle at different temperatures is realized.
The first object of the invention is to provide a nonaqueous electrolytic solution, which comprises an electrolyte lithium salt, a nonaqueous organic solvent and an additive, wherein the additive comprises lithium bis (oxalato) borate and lithium difluoro (oxalato) phosphate;
wherein the lithium bis (oxalato) borate accounts for 0.5-2% of the total mass of the electrolyte, and the lithium difluoro bis (oxalato) phosphate accounts for 0.5-2% of the total mass of the electrolyte.
Further, the additive also comprises one or more of 1, 3-propane sultone PS, fluoroethylene carbonate FEC, ethylene sulfate DTD and vinylene carbonate VC.
Further, the content of the electrolyte lithium salt is 10-20% of the total mass of the electrolyte.
Further, the electrolyte lithium salt is selected from lithium hexafluorophosphate (LiPF)6) Lithium difluorophosphate (LiPO)2F2) Lithium bis (fluorosulfonylimide) (LiFSI) or bis (trifluoro-phosphonium) compoundLithium methanesulfonamide (LiTFSI) and lithium tetrafluoroborate (LiBF)4) One or more of them.
Further, the non-aqueous organic solvent is selected from one or more of a linear carbonate solvent, a cyclic carbonate solvent, a carboxylic acid ester solvent, and a fluorinated carbonate solvent.
Further, the straight-chain carbonate solvent is selected from one or more of ethyl methyl carbonate, dimethyl carbonate and diethyl carbonate; the cyclic carbonate solvent is selected from one or more of ethylene carbonate and propylene carbonate; the carboxylic ester solvent is selected from one or more of ethyl acetate, ethyl propionate, methyl propionate, propyl butyrate and propyl acetate; the fluorinated carbonate solvent is selected from one or more of fluorinated ethylene carbonate, 1, 2-difluoroethylene carbonate, methyl trifluoroethyl carbonate and bis trifluoroethyl carbonate.
The second purpose of the invention is to provide the application of the electrolyte in the preparation of a lithium ion battery, wherein the charging voltage of the lithium ion battery is less than 5.5V.
A third object of the present invention is to provide a lithium ion battery comprising: a positive electrode, a negative electrode, a separator between the positive electrode and the negative electrode, and the electrolyte;
the positive electrode includes a positive electrode active material;
the negative electrode comprises a negative current collector and a negative diaphragm arranged on the negative current collector, and the negative diaphragm comprises a negative active material, a negative conductive agent and a binder.
Further, the positive active material is selected from one or more of lithium cobaltate, lithium nickelate, lithium manganate, lithium vanadate, lithium iron phosphate, lithium iron manganese phosphate, lithium nickel manganese oxide, lithium cobalt manganese manganate, lithium-rich manganese-based material and ternary positive material, and the structural formula of the ternary positive material is LiNi1-x-y-zCoxMnyAlzO2Wherein x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than or equal to 0 and less than or equal to 1, and x + y + z is more than or equal to 0 and less than or equal to 1.
Further, the negative active material is selected from one or more of artificial graphite, natural graphite, silicon-oxygen compound, silicon-based alloy and active carbon; the negative electrode conductive agent is selected from one or more of acetylene black, conductive carbon black, carbon fiber, carbon nanotube and Ketjen black.
Further, the kind of the diaphragm is not particularly limited and may be selected according to actual requirements. Preferably, the diaphragm comprises a base film and a nano alumina coating coated on the base film, wherein the base film is at least one of PP, PE and PET, and the thickness of the nano alumina coating is 1.0-6.0 μm.
In the invention, the high-voltage non-aqueous electrolyte refers to a non-aqueous electrolyte suitable for a lithium ion battery under a high-voltage condition, and the high voltage specifically refers to a charging voltage of 4.1-5.5V.
The matching principle and the action of all substances in the lithium ion battery electrolyte are as follows: in the process of charging and discharging of the lithium ion battery, main components and additives in the electrolyte can be decomposed and polymerized on the surfaces of a positive electrode and a negative electrode, and a polymer with large molecular weight can be separated out on the surface of the electrode and wraps the generated inorganic lithium salt to form a solid electrolyte membrane which can isolate the electrolyte and can conduct ions. The electrolyte formed by the electrolyte solvent is thick and loose, and is difficult to protect and isolate the electrolyte, so that the electrolyte can be thickened continuously, the battery impedance is increased, and continuous electrolyte loss is brought. The lithium bis (oxalato) borate and the lithium difluoro bis (oxalato) phosphate are lithium salt additives, the coordination number of central atoms of the lithium bis (oxalato) borate and the lithium difluoro bis (oxalato) phosphate is too large, and the lithium bis (oxalato) borate and the lithium difluoro bis (oxalato) phosphate are easy to be bonded with electrolyte membranes with similar groups around again, so that the electrolyte membranes are prevented from continuously growing, stable P, B end groups are formed, the thickness and stability of electrode surface membranes are controlled, and the performances of low impedance growth and long circulation at different.
By the scheme, the invention at least has the following advantages:
according to the invention, lithium salt additives, namely lithium bis (oxalato) borate and lithium difluoro (oxalato) phosphate are added, central atoms of the lithium bis (oxalato) borate and the lithium difluoro (oxalato) phosphate are matched with each other and are re-bonded with electrolyte membranes with similar groups around, so that the continuous growth of the electrolyte membranes is prevented, a stable P, B terminal group is formed, the thickness and stability of electrode surface membranes are controlled, and the performances of low impedance growth and long circulation at different temperatures are realized.
The foregoing is a summary of the present invention, and in order to provide a clear understanding of the technical means of the present invention and to be implemented in accordance with the present specification, the following is a preferred embodiment of the present invention and is described in detail below.
Detailed Description
In the present invention, the electrolyte solution includes an electrolyte lithium salt selected from lithium hexafluorophosphate (LiPF), a non-aqueous organic solvent and an additive6) Lithium difluorophosphate (LiPO)2F2) Lithium bis (fluorosulfonylimide) (LiFSI), lithium bis (trifluoromethanesulfonylimide) (LiTFSI), and lithium tetrafluoroborate (LiBF)4) The non-aqueous organic solvent is selected from one or more of a linear carbonate solvent, a cyclic carbonate solvent, a carboxylic ester solvent and a fluorinated carbonate solvent, and the additive comprises 1, 3-propanesultone PS, lithium bis (oxalato) borate LiBOB and lithium difluoro (oxalato) phosphate LiODFP; the lithium bis (oxalate) borate accounts for 0.5-3% of the total mass of the electrolyte, the lithium difluoro (oxalate) phosphate accounts for 0.5-2% of the total mass of the electrolyte, and the lithium difluoro (oxalate) phosphate further comprises one or more of fluoroethylene carbonate FEC, ethylene sulfate DTD and vinylene carbonate VC.
The following examples are given to further illustrate the embodiments of the present invention. The following examples are intended to illustrate the invention but are not intended to limit the scope of the invention.
The lithium ion secondary battery of the present invention is prepared by:
LiNi as positive electrode active material0.5Co0.2Mn0.3O2(LNCM), conductive agent acetylene black and adhesive polyvinylidene fluoride (PVDF) are fully stirred and mixed uniformly in an N-methyl pyrrolidone solvent system according to the mass ratio of 95: 3: 2, then the mixture is coated on an aluminum foil to be dried and cold-pressed, and a positive pole piece is obtained, wherein the compaction density of the positive pole piece is 3.45g/cm3。
Mixing graphite as negative active material, acetylene black as conducting agent, Styrene Butadiene Rubber (SBR) as adhesive and sodium carboxymethyl cellulose (CMC) as thickener in the weight ratio of 96 to 2The mixture is fully stirred and mixed uniformly in a deionized water solvent system in a ratio of 1: 1, and then the mixture is coated on a Cu foil for drying and cold pressing to obtain a negative pole piece, wherein the compaction density of the negative pole piece is 1.65g/cm3。
Polyethylene (PE) with the thickness of 9 mu m is taken as a base film, and a nano aluminum oxide coating layer with the thickness of 3 mu m is coated on the base film to obtain the diaphragm.
And stacking the positive and negative pole pieces and the diaphragm made of polyethylene in a negative pole, diaphragm, positive pole and diaphragm mode, and ending with the negative pole to obtain the bare cell.
And (3) carrying out hot pressing on the naked electric core to ensure that polyvinylidene fluoride (PVDF) on the surface of the diaphragm bonds the pole pieces together. And (3) welding the lugs of the hot-pressed bare cell, placing the bare cell in an aluminum plastic film with a punched pit, and carrying out hot-melt packaging to obtain the pre-packaged battery with a liquid injection port. And (3) placing the pre-packaged battery in a vacuum furnace for fully baking and drying, injecting corresponding electrolyte from the liquid injection port, and packaging the liquid injection port in a vacuum environment to obtain the secondary battery.
The secondary battery of the present invention can be tested by the following method:
(1) initial discharge capacity and cycle test of secondary battery
The prepared battery is aged and placed on a clamp, the activated battery is charged to 4.3V at 25 ℃ by using a current of 1C, the voltage is constant to 0.05C, the battery is discharged to 2.8V by using 1C, and the discharge capacity is recorded. And recording initial DCR of the battery after the first circle of discharge, then performing a cycle test until the discharge capacity of the battery is 80% of the first circle of capacity, and recording the DCR, the increase rate of the DCR, the number of turns of the battery reaching 80% SOH (state of health of the battery) and the change of gas production volume of the battery after the cycle is finished.
Wherein the change in the direct current resistance of the secondary battery and the volume of the generated gas are measured by the following methods, respectively:
(i) direct Current Resistance (DCR) test of secondary battery
When the battery is discharged to 50% SOC (state of charge, reflecting the residual capacity of the battery) at a specified temperature by 1C current, the current is increased to 4C and kept for 30s, the difference between the updated stable voltage and the original platform voltage is detected, and the ratio of the value to the 3C current value is the direct current resistance of the battery. And comparing the DCR after the cycle is ended with the DCR at the beginning of the cycle to obtain the increase rate of the DCR.
(ii) Volume change test of gas generated by secondary battery
Fixing the secondary battery with a string, completely soaking the secondary battery in water at 25 ℃, recording the weight difference before and after soaking, and converting the weight difference into the volume difference according to the density of the water at 25 ℃.
(2) Capacity recovery test of secondary battery at 60 deg.C
After aging treatment of examples 5, 6, 7 and comparative example 2, the activated battery was charged to 4.3V at 25 ℃ with a current of 1C and was constant-voltage to a current of 0.05C. The secondary battery was placed in an environment at 60 ℃ for 60 days, and the capacity recovery rate was recorded for 60 days.
(3) Cycle test of secondary battery at 60 deg.C
After aging treatment of examples 5, 6 and 7 and comparative examples 2 and 3, the activated cell was charged to 4.25V at 60 ℃ with a current of 1C, and was constant-voltage to a current of 0.05C, and then discharged to 3.0V at 1C, and the discharge capacity was recorded. And recording initial DCR of the battery after the first circle of discharge, then performing a cycle test until the discharge capacity of the battery is 80% of the first circle of capacity, and recording the DCR, the increase rate of the DCR and the gas production volume change of the battery after the cycle is finished.
Low temperature discharge test
The full-state battery after capacity separation was discharged to 3.0V at 25 ℃ at 1C, and the initial discharge capacity was recorded as DC (25 ℃). Then, the mixture was charged to 4.2V at 25 ℃ at a constant current and a constant voltage of 1C, and the current was cut off at 0.05C. The temperature is reduced to minus 20 ℃ and the mixture is kept for 4 hours, then the mixture is discharged to 3.0V at 1C, and the discharge capacity DC (-20 ℃) is recorded. The low-temperature discharge capacity retention rate was 100% DC (-20 ℃)/DC (25 ℃).
The corresponding electrolyte above was prepared according to the following examples:
example 1:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to obtain a non-aqueous organic solvent, and adding 12% of LiPF6 and 1.5% of LiPO which are calculated according to the total mass of the finished electrolyte2F21% LiFSI, 0.5% VC, 0.5% PS, 0.5% LiBOB and 0.5% LiODFP, and uniformly mixing to obtain the electrolyte.
Comparative example 1:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to obtain a non-aqueous organic solvent, and adding 12% of LiPF6 and 1.5% of LiPO which are calculated according to the total mass of the finished electrolyte2F21% LiFSI, 2% VC and 0.5% PS, and uniformly mixing to obtain the electrolyte.
Comparative example 2:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to obtain a non-aqueous organic solvent, and adding 12% of LiPF6 and 1.5% of LiPO which are calculated according to the total mass of the finished electrolyte2F21% LiFSI, 0.5% VC, 0.5% PS and 1% LiBOB, and uniformly mixing to obtain the electrolyte.
Comparative example 3:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to obtain a non-aqueous organic solvent, and adding 12% of LiPF6 and 1.5% of LiPO which are calculated according to the total mass of the finished electrolyte2F21% LiFSI, 0.5% VC, 0.5% PS and 1% LiODFP, and uniformly mixing to obtain the electrolyte.
The results of the electrical property tests of the different lithium ion batteries of example 1 and comparative examples 1 to 3 are shown in table 1, and the charge cut-off voltage of each lithium ion secondary battery was 4.4V. The result shows that only LiBOB and LiODFP are added and used in a matching way, the lithium bis (oxalato) borate and the lithium difluoro bis (oxalato) phosphate are matched with central atoms of the lithium bis (oxalato) borate and the lithium difluoro bis (oxalato) phosphate to be re-bonded with electrolyte membranes with similar groups around, so that the electrolyte membranes are prevented from continuously growing, stable P, B end groups are formed, the thickness and the stability of the surface membranes of the electrodes are controlled, and the performances of low impedance growth and long circulation at different temperatures are realized.
TABLE 1
Example 2:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to obtain a non-aqueous organic solvent, and adding 12% of LiPF6 and 1% of LiPO which are calculated according to the total mass of the finished electrolyte2F21% LiFSI, 1% LiTFSI, 1.5% DTD, 0.5% VC, 1% PS, 0.5% LiBOB and 0.5% LiODFP, and uniformly mixing to obtain the electrolyte.
Example 3:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 6 parts of EMC, 1 part of DEC and 4 parts of PC/Add into a non-aqueous organic solvent, and adding 13% LiPF6 and 1% LiPO which are obtained according to the total mass of the finished electrolyte2F2、0.4％LiBF40.5% of DTD, 0.5% of VC, 1% of PS, 0.5% of LiBOB and 0.5% of LiODFP, and uniformly mixing to obtain the electrolyte.
Example 4:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to obtain a non-aqueous organic solvent, and adding 13% of LiPF6 and 1% of LiPO which are calculated according to the total mass of the finished electrolyte2F2And 3% of FEC, 1% of PS, 0.5% of LiBOB and 0.5% of LiODFP, and uniformly mixing to obtain the electrolyte.
Comparative example 4:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to obtain a non-aqueous organic solvent, and adding 13% of LiPF6 and 1% of LiPO which are calculated according to the total mass of the finished electrolyte2F23% of FEC, 1% of PS and 0.5% of LiODFP, and uniformly mixing to obtain the electrolyte.
Comparative example 5:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 5 parts of EMC and 2 parts of DEC to form a non-aqueous organic solvent, and adding 4% LiPF6, 2% LiFSI, 1% LiTFSI and 0.1% LiBF which are obtained according to the total mass of the finished electrolyte4、0.5％VC、1％PS、5％And mixing the LiBOB and 5% LiODFP uniformly to obtain the electrolyte.
Comparative example 6:
the preparation steps of the electrolyte are as follows:
mixing 3 parts of EC, 6 parts of EMC, 1 part of DEC and 4 parts of PC/Add into a non-aqueous organic solvent, and adding 13.5 percent LiPF6 and 1 percent LiPO which are calculated according to the total mass of the finished electrolyte2F2、0.4％LiBF40.5% of DTD, 0.5% of VC and 0.5% of PS are uniformly mixed to obtain the electrolyte.
The results of the electrical property tests of the different lithium ion batteries of examples 2 to 4 and comparative examples 4 to 6 are shown in table 2, and the charge cut-off voltage of each lithium ion secondary battery was 4.4V. The result shows that the good performance of low impedance growth and long cycle can be achieved only by adding LiBOB and LiODFP together, and the dosage of the additive also needs to be limited within a certain range to play a good role.
TABLE 2 test results of electrical properties of different lithium ion batteries
The above is only a preferred embodiment of the present invention, and is not intended to limit the present invention, it should be noted that, for those skilled in the art, many modifications and variations can be made without departing from the technical principle of the present invention, and these modifications and variations should also be regarded as the protection scope of the present invention.
Claims (10)
1. A nonaqueous electrolytic solution comprising an electrolyte lithium salt, a nonaqueous organic solvent and an additive, characterized in that the additive comprises lithium bis (oxalato) borate and lithium bis (oxalato) phosphate;
wherein the lithium bis (oxalato) borate accounts for 0.5-2% of the total mass of the electrolyte, and the lithium difluoro bis (oxalato) phosphate accounts for 0.5-2% of the total mass of the electrolyte.
2. The nonaqueous electrolytic solution of claim 1, wherein the additive further comprises one or more of 1, 3-propanesultone, fluoroethylene carbonate, ethylene sulfate, and vinylene carbonate.
3. The nonaqueous electrolytic solution of claim 1, wherein the content of the electrolytic lithium salt is 10 to 20% by mass of the total mass of the electrolytic solution.
4. The nonaqueous electrolytic solution of claim 1, wherein the electrolyte lithium salt is one or more selected from lithium hexafluorophosphate, lithium difluorophosphate, lithium bis-fluorosulfonylimide, lithium bis-trifluoromethanesulfonylimide, and lithium tetrafluoroborate.
5. The nonaqueous electrolytic solution of claim 1, wherein the nonaqueous organic solvent is one or more selected from a linear carbonate-based solvent, a cyclic carbonate-based solvent, a carboxylic acid-based solvent, and a fluorinated carbonate-based solvent.
6. The nonaqueous electrolytic solution of claim 5, wherein the linear carbonate-based solvent is one or more selected from ethyl methyl carbonate, dimethyl carbonate, and diethyl carbonate; the cyclic carbonate solvent is selected from one or more of ethylene carbonate and propylene carbonate; the carboxylic ester solvent is selected from one or more of ethyl acetate, ethyl propionate, methyl propionate, propyl butyrate and propyl acetate; the fluorinated carbonate solvent is selected from one or more of fluorinated ethylene carbonate, 1, 2-difluoroethylene carbonate, methyl trifluoroethyl carbonate and bis trifluoroethyl carbonate.
7. Use of the nonaqueous electrolytic solution according to any one of claims 1 to 6 for producing a lithium ion battery, wherein a charging voltage of the lithium ion battery is 5.5V or less.
8. A lithium ion battery, comprising: a positive electrode, a negative electrode, a separator between the positive electrode and the negative electrode, and the nonaqueous electrolytic solution of any one of claims 1 to 6;
the positive electrode includes a positive electrode active material;
the negative electrode comprises a negative current collector and a negative diaphragm arranged on the negative current collector, and the negative diaphragm comprises a negative active material, a negative conductive agent and a binder.
9. The lithium ion battery of claim 8, wherein the positive active material is selected from one or more of lithium cobaltate, lithium nickelate, lithium manganate, lithium vanadate, lithium iron phosphate, lithium iron manganese phosphate, lithium nickel manganate, lithium cobalt manganate, lithium manganese rich-based material and ternary positive material, and the ternary positive material has a structural formula of LiNi1-x-y-zCoxMnyAlzO2Wherein x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than or equal to 0 and less than or equal to 1, and x + y + z is more than or equal to 0 and less than or equal to 1.
10. The lithium ion battery of claim 8, wherein the negative active material is selected from one or more of artificial graphite, natural graphite, silicon-oxygen compound, silicon-based alloy and activated carbon; the negative electrode conductive agent is selected from one or more of acetylene black, conductive carbon black, carbon fiber, carbon nanotube and Ketjen black.
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