CN111129586A - A high-voltage lithium cobalt oxide lithium ion battery non-aqueous electrolyte and lithium ion battery - Google Patents
A high-voltage lithium cobalt oxide lithium ion battery non-aqueous electrolyte and lithium ion battery Download PDFInfo
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- CN111129586A CN111129586A CN201911325582.XA CN201911325582A CN111129586A CN 111129586 A CN111129586 A CN 111129586A CN 201911325582 A CN201911325582 A CN 201911325582A CN 111129586 A CN111129586 A CN 111129586A
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- ion battery
- lithium ion
- lithium
- cobalt oxide
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- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 43
- FLAFBICRVKZSCF-UHFFFAOYSA-N [Li].[Co]=O.[Li] Chemical compound [Li].[Co]=O.[Li] FLAFBICRVKZSCF-UHFFFAOYSA-N 0.000 title claims abstract description 25
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 18
- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 18
- 239000003792 electrolyte Substances 0.000 claims abstract description 44
- 239000000654 additive Substances 0.000 claims abstract description 38
- 230000000996 additive effect Effects 0.000 claims abstract description 32
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 17
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 17
- 239000012948 isocyanate Substances 0.000 claims abstract description 15
- 150000002513 isocyanates Chemical class 0.000 claims abstract description 15
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 14
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 14
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 10
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 14
- 239000000203 mixture Substances 0.000 claims description 13
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 8
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 claims description 8
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 7
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 7
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 7
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 4
- 229940008841 1,6-hexamethylene diisocyanate Drugs 0.000 claims description 4
- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 claims description 4
- VTHRQKSLPFJQHN-UHFFFAOYSA-N 3-[2-(2-cyanoethoxy)ethoxy]propanenitrile Chemical compound N#CCCOCCOCCC#N VTHRQKSLPFJQHN-UHFFFAOYSA-N 0.000 claims description 4
- RRAMGCGOFNQTLD-UHFFFAOYSA-N hexamethylene diisocyanate Chemical compound O=C=NCCCCCCN=C=O RRAMGCGOFNQTLD-UHFFFAOYSA-N 0.000 claims description 4
- GSLTVFIVJMCNBH-UHFFFAOYSA-N 2-isocyanatopropane Chemical compound CC(C)N=C=O GSLTVFIVJMCNBH-UHFFFAOYSA-N 0.000 claims description 3
- WUDNUHPRLBTKOJ-UHFFFAOYSA-N ethyl isocyanate Chemical compound CCN=C=O WUDNUHPRLBTKOJ-UHFFFAOYSA-N 0.000 claims description 3
- WARQUFORVQESFF-UHFFFAOYSA-N isocyanatoethene Chemical compound C=CN=C=O WARQUFORVQESFF-UHFFFAOYSA-N 0.000 claims description 3
- -1 lithium hexafluorophosphate Chemical compound 0.000 claims description 3
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 claims description 3
- 238000004804 winding Methods 0.000 claims description 3
- 125000000217 alkyl group Chemical group 0.000 claims description 2
- 125000003118 aryl group Chemical group 0.000 claims description 2
- 150000005678 chain carbonates Chemical class 0.000 claims description 2
- 150000005676 cyclic carbonates Chemical class 0.000 claims description 2
- KQWGXHWJMSMDJJ-UHFFFAOYSA-N cyclohexyl isocyanate Chemical compound O=C=NC1CCCCC1 KQWGXHWJMSMDJJ-UHFFFAOYSA-N 0.000 claims description 2
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims description 2
- 125000003709 fluoroalkyl group Chemical group 0.000 claims description 2
- LNLFLMCWDHZINJ-UHFFFAOYSA-N hexane-1,3,6-tricarbonitrile Chemical compound N#CCCCC(C#N)CCC#N LNLFLMCWDHZINJ-UHFFFAOYSA-N 0.000 claims description 2
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 claims description 2
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 claims description 2
- 150000007942 carboxylates Chemical class 0.000 claims 1
- 239000008151 electrolyte solution Substances 0.000 claims 1
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 abstract description 18
- 239000007774 positive electrode material Substances 0.000 abstract description 14
- 229910001429 cobalt ion Inorganic materials 0.000 abstract description 4
- XLJKHNWPARRRJB-UHFFFAOYSA-N cobalt(2+) Chemical compound [Co+2] XLJKHNWPARRRJB-UHFFFAOYSA-N 0.000 abstract description 4
- 230000000052 comparative effect Effects 0.000 description 7
- 150000001875 compounds Chemical class 0.000 description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- 238000007599 discharging Methods 0.000 description 4
- 230000014759 maintenance of location Effects 0.000 description 4
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 230000007547 defect Effects 0.000 description 3
- 238000009472 formulation Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 239000012528 membrane Substances 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 238000011056 performance test Methods 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- 239000004698 Polyethylene Substances 0.000 description 2
- 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 2
- 239000006230 acetylene black Substances 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 239000010405 anode material Substances 0.000 description 2
- 229910021383 artificial graphite Inorganic materials 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 229920003123 carboxymethyl cellulose sodium Polymers 0.000 description 2
- 229940063834 carboxymethylcellulose sodium Drugs 0.000 description 2
- 229910017052 cobalt Inorganic materials 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 238000005056 compaction Methods 0.000 description 2
- 239000006258 conductive agent Substances 0.000 description 2
- 230000002950 deficient Effects 0.000 description 2
- 238000004090 dissolution Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 238000010030 laminating Methods 0.000 description 2
- 239000007773 negative electrode material Substances 0.000 description 2
- 238000002161 passivation Methods 0.000 description 2
- 229920000573 polyethylene Polymers 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- YKYONYBAUNKHLG-UHFFFAOYSA-N propyl acetate Chemical compound CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical class N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 description 1
- MEKOFIRRDATTAG-UHFFFAOYSA-N 2,2,5,8-tetramethyl-3,4-dihydrochromen-6-ol Chemical compound C1CC(C)(C)OC2=C1C(C)=C(O)C=C2C MEKOFIRRDATTAG-UHFFFAOYSA-N 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910010743 LiFeSi Inorganic materials 0.000 description 1
- 229910001290 LiPF6 Inorganic materials 0.000 description 1
- 229910012265 LiPO2F2 Inorganic materials 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 229910020219 SiOw Inorganic materials 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 150000001733 carboxylic acid esters Chemical class 0.000 description 1
- 229940125904 compound 1 Drugs 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000010828 elution Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 125000001153 fluoro group Chemical group F* 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- DUDXQIXWPJMPRQ-UHFFFAOYSA-N isocyanatomethylcyclohexane Chemical compound O=C=NCC1CCCCC1 DUDXQIXWPJMPRQ-UHFFFAOYSA-N 0.000 description 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 238000009517 secondary packaging Methods 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 239000002153 silicon-carbon composite material Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 229910001428 transition metal ion Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or 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 discloses a high-voltage lithium cobaltate lithium ion battery non-aqueous electrolyte, which comprises a non-aqueous organic solvent, electrolyte lithium salt and an additive, wherein the additive comprises the following components in percentage by mass in the electrolyte: 0.5-1.0% of isocyanate additive and 0.5-20% of other additives. The invention also discloses a high-voltage lithium cobalt oxide lithium ion battery. The isocyanate additive in the non-aqueous electrolyte of the high-voltage lithium cobalt oxide lithium ion battery can form a film on the positive electrode, inhibit the positive electrode material from being corroded by hydrofluoric acid in the electrolyte, inhibit the positive electrode material structure from collapsing and cobalt ions from dissolving out caused by the hydrofluoric acid, and improve the electrochemical performance of the high-voltage lithium cobalt oxide lithium ion battery.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a high-voltage lithium cobaltate lithium ion battery non-aqueous electrolyte and a lithium ion battery.
Background
The lithium ion battery has the advantages of high working voltage, high energy density, long service life, wide working temperature range, environmental friendliness and the like, and is widely applied to the fields of 3C digital products, electric tools, electric automobiles, aerospace and the like. With the demand for batteries becoming higher and higher, the development trend of batteries is light, thin and high energy density, especially for 3C digital products, such as mobile phone batteries, tablet computers and camera devices.
In order to increase the energy density of a lithium ion battery, a common measure is to increase the charge cut-off voltage of a positive electrode material, such as a commercial lithium cobalt oxide battery voltage from 4.2V → 4.35V → 4.4V → 4.45V → 4.48V → 4.5V. However, the positive electrode material has certain defects under high voltage, for example, the high-voltage positive electrode active material has strong oxidizability in a lithium-deficient state, and the electrolyte is easily oxidized and decomposed to generate a large amount of gas and heat; in addition, the high-voltage positive electrode active material itself is also unstable in a lithium-deficient state, and is prone to some side reactions, such as oxygen release, transition metal ion elution, and the like.
Chinese patent CN109755636A discloses a high-temperature high-pressure safety lithium ion battery electrolyte and a lithium ion battery, wherein the lithium ion battery electrolyte comprises lithium salt, a non-aqueous organic solvent and an additive, and the additive comprises an isocyanate additive, a film-forming additive and a fluoro-flame retardant additive. The lithium ion battery electrolyte can form a stable SEI film on the surface of an electrode material by adding the first type of isocyanate additive and the second type of film forming additive, so that the lithium ion battery electrolyte is beneficial to ion conduction and can inhibit the decomposition of the electrolyte; and by adding a third type of fluorinated flame retardant, F atoms can form a film on an electrode interface, and the intermolecular force can be reduced, the viscosity of the electrolyte can be reduced, and the conductivity of the electrolyte can be improved. The components have synergistic effect, so that the battery has good high-temperature storage performance, normal-temperature cycle performance and high-temperature cycle performance under high voltage, and has no potential safety hazard. The defect is that the additive can not be oxidized at the interface of the lithium cobaltate material of the positive electrode to form a passive film.
Disclosure of Invention
In order to overcome the defects of the background technology, the invention provides the high-voltage lithium cobalt oxide lithium ion battery non-aqueous electrolyte and the lithium ion battery, wherein the additive in the high-voltage lithium cobalt oxide lithium ion battery non-aqueous electrolyte can form a film on the positive electrode, inhibit the corrosion of the positive electrode material by hydrofluoric acid in the electrolyte, inhibit the collapse of the positive electrode material structure and the dissolution of cobalt ions caused by the hydrofluoric acid, and improve the electrochemical performance of the high-voltage lithium cobalt oxide lithium ion battery.
In order to achieve the purpose, the invention adopts the technical scheme that: a high-voltage lithium cobalt oxide lithium ion battery non-aqueous electrolyte comprises a non-aqueous organic solvent, electrolyte lithium salt and an additive, wherein the additive comprises the following components in percentage by mass in the electrolyte:
0.5 to 1.0 percent of isocyanate additive
0.5 to 20 percent of other additives
As a preferred embodiment of the present invention, the isocyanate additive has a structural formula shown in formula (I) or formula (II):
wherein R, R2，R3It is an alkyl group, a fluoroalkyl group, a phenyl group or an aryl group.
The isocyanate additive is more preferably at least one of 1, 6-hexamethylene diisocyanate, vinyl isocyanate, isopropyl isocyanate, cyclohexyl isocyanate, p-benzyl isocyanate and ethyl isocyanate. Their structural formulae are shown below:
as a preferred embodiment of the present invention, the electrolyte lithium salt is a mixture of lithium hexafluorophosphate, lithium difluorosulfonimide and lithium difluorophosphate.
In a preferred embodiment of the present invention, the electrolyte lithium salt is contained in the electrolyte in an amount of 13.5 to 17.5% by mass.
As a preferred embodiment of the present invention, the other additive is one or more of fluoroethylene carbonate (FEC), 1,3, 6-Hexanetricarbonitrile (HTCN), 1, 3-Propanesultone (PS), Adiponitrile (ADN), vinyl sulfate (DTD), Succinonitrile (SN), 1, 2-bis (cyanoethoxy) ethane (done). More preferably, the other additive is a mixture of fluoroethylene carbonate (FEC), 1, 3-Propane Sultone (PS), Adiponitrile (ADN), 1, 2-bis (cyanoethoxy) ethane (DENE).
As a preferred embodiment of the present invention, the non-aqueous organic solvent may be one or a mixture of more of cyclic carbonates, chain carbonates, and carboxylic acid esters. The non-aqueous organic solvent is preferably one or more of Ethylene Carbonate (EC), Propylene Carbonate (PC), diethyl carbonate (DEC), ethyl acetate, n-propyl acetate, Ethyl Propionate (EP) and Propyl Propionate (PP). The non-aqueous organic solvent is more preferably a mixture of ethylene carbonate, propylene carbonate, diethyl carbonate, ethyl propionate and propyl propionate.
The invention also provides a high-voltage lithium cobalt oxide lithium ion battery which comprises a battery core formed by laminating or winding the positive plate, the isolating membrane and the negative plate and the high-voltage lithium cobalt oxide lithium ion battery electrolyte.
Preferably, the positive active material of the positive plate is a lithium cobaltate active material, and the compaction density of the positive plate is 4.0-4.2 g/cm3。
Preferably, the negative active material of the negative electrode sheet is artificial graphite, natural graphite, or SiOwThe silicon-carbon composite material is compounded with graphite, wherein w is more than 1 and less than 2, and the compaction density of the negative plate is 1.5-1.70 g/cm3。
The inventor finds out through a large number of experiments that the isocyanate additive can not be reduced to form a film on the graphite interface of the negative electrode, but is oxidized to form a passivation film on the lithium cobaltate material interface of the positive electrode, so that the electrochemical performance of the lithium cobaltate high-voltage battery is improved. Therefore, the additive in the non-aqueous electrolyte of the high-voltage lithium cobalt oxide lithium ion battery can form a film on the positive electrode, inhibit the positive electrode material from being corroded by hydrofluoric acid in the electrolyte, inhibit the positive electrode material structure from collapsing and cobalt ions from dissolving out caused by the hydrofluoric acid, and improve the electrochemical performance of the high-voltage lithium cobalt oxide lithium ion battery.
Compared with the prior art, the invention has the advantages that:
1. the isocyanate additive in the high-voltage lithium cobalt oxide lithium ion battery electrolyte can form a film on a positive electrode, inhibit the positive electrode material from being corroded by hydrofluoric acid in the electrolyte and inhibit the positive electrode material structure from collapsing and cobalt ions from dissolving out caused by the hydrofluoric acid.
2. The invention improves the infiltration difficulty in a high-voltage cobalt acid lithium battery system by optimizing the combination and proportion of the solvent, and further improves the electrochemical performance of the lithium ion battery by introducing the mixed lithium salt.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It is to be understood that the following description is only illustrative of the present invention and is not to be construed as limiting the present invention
The isocyanate-based additives of the examples are characterized by the following structural formula:
the compound (1) is 1, 6-hexamethylene diisocyanate,
the compound (2) is vinyl isocyanate,
the compound (3) is isopropyl isocyanate,
the compound (4) is cyclohexyl methyl isocyanate,
the compound (5) is p-phenylmethyl isocyanate,
the compound (6) is ethyl isocyanate
Their structural formulae are shown below:
example 1
Preparing an electrolyte: in a glove box filled with argon, Ethylene Carbonate (EC), Propylene Carbonate (PC), diethyl carbonate (DEC), Ethyl Propionate (EP) and Propyl Propionate (PP) were mixed in a mass ratio of EC: PC: DEC: EP: PP 20: 10: 20: 20: 30 to obtain a mixed solution, and then slowly adding the mixed solutionInto LiPF6LiFeSi and LiPO2F2The mixed lithium salt of the composition was dissolved to prepare a solution containing the mixed lithium salt, and then compound (1) was added to the solution containing the mixed lithium salt, followed by addition of FEC, PS, ADN, and done, and stirring was performed to completely dissolve them, thereby obtaining an electrolyte of example 1. The mass percent of the mixed lithium salt in the electrolyte is 15.5%, the mass percent of the compound (1) in the electrolyte is 1.0%, the mass percent of the FEC in the electrolyte is 8%, the mass percent of the PS in the electrolyte is 5%, the mass percent of the ADN in the electrolyte is 2%, and the mass percent of the DENE in the electrolyte is 1%. The electrolyte formulation is shown in table 1.
Examples 2 to 10
Examples 2-10 are also specific examples of electrolyte preparation, and the parameters and preparation method are the same as example 1 except for the parameters in Table 1. The electrolyte formulation is shown in table 1.
Comparative example 1
In comparative example 1, the parameters and preparation method were the same as in example 1 except for the parameters shown in Table 1. The electrolyte formulation is shown in table 1.
TABLE 1 composition ratios of respective components of electrolytes of examples 1 to 10 and comparative example 1
Note: the concentration of the lithium salt is the mass percentage content in the electrolyte;
the content of the isocyanate additive is the mass percentage content in the electrolyte;
the content of each component in other additives is the mass percentage content in the electrolyte;
the proportion of each component in the non-aqueous organic solvent is volume ratio.
Lithium ion battery performance testing
Preparing a lithium ion battery:
mixing a positive electrode active material lithium cobaltate, a conductive agent acetylene black and a binder polyvinylidene fluoride (PVDF) according to a mass ratio of 96.5: 3: 1.5 fully stirring and uniformly mixing in an N-methyl pyrrolidone solvent system, coating on an aluminum foil, drying, and cold pressing to obtain the positive plate.
Preparing negative active material artificial graphite, conductive agent acetylene black, binder Styrene Butadiene Rubber (SBR), and thickener carboxymethylcellulose sodium (CMC) according to a mass ratio of 96: 2: 1: 1, fully stirring and uniformly mixing in a deionized water solvent system, coating on a copper foil, drying, and cold pressing to obtain the negative plate.
Polyethylene (PE) is used as a base film, and a nano aluminum oxide coating is coated on the base film to be used as an isolating film.
And sequentially laminating the positive plate, the isolating membrane and the negative plate, winding the positive plate, the isolating membrane and the negative plate along the same direction to obtain a bare cell, placing the bare cell in an outer package, injecting the electrolyte prepared in the examples 1-10 and the comparative example 1, and carrying out the procedures of packaging, shelving at 45 ℃, high-temperature clamp formation, secondary packaging, capacity grading and the like to obtain the high-voltage lithium cobalt oxide lithium ion battery.
The following performance tests were performed on the batteries of examples 1-10 and comparative example 1, respectively, and the test results are shown in table 2, wherein:
1) and (3) testing the normal-temperature cycle performance of the cobalt acid lithium battery: and at the temperature of 25 ℃, charging the battery with the capacity divided to 4.45V at a constant current and a constant voltage of 0.7C, stopping the current at 0.02C, then discharging the battery to 3.0V at a constant current of 0.7C, and circulating the battery according to the above steps, and calculating the capacity retention rate of 500 cycles after 500 cycles of charging/discharging. The calculation formula is as follows:
the 500 th cycle capacity retention ratio (%) (500 th cycle discharge capacity/first cycle discharge capacity) × 100%.
2) Testing the residual rate of the 85 ℃ constant-temperature storage capacity of the lithium cobaltate battery: firstly, the battery is circularly charged and discharged for 1 time (4.45V-3.0V) at the normal temperature at 0.7C, and the discharge capacity C before the battery is stored is recorded0Then the battery is charged to a full state of 4.45V at constant current and constant voltage, and then the battery is put into a thermostat with the temperature of 85 ℃ for storage for 4hTaking out the battery after the storage is finished; after the battery is cooled for 24 hours at room temperature, the battery is discharged to 3.0V at a constant current of 0.7C again, and the discharge capacity C after the battery is stored is recorded1And calculating the capacity residual rate of the battery after being stored for 4 hours at the constant temperature of 85 ℃, wherein the calculation formula is as follows:
after being stored for 4 hours at constant temperature of 85 ℃, the capacity residual rate is C1/C0*100％。
3) And (3) testing 45 ℃ cycle performance of the lithium cobaltate battery: and (3) at the temperature of 45 ℃, charging the battery with the capacity divided to 4.45V at a constant current and a constant voltage of 0.7C, stopping the current at 0.02C, then discharging the battery to 3.0V at a constant current of 0.7C, and circulating the battery according to the above steps, and calculating the capacity retention ratio of the battery in the 300 th cycle after 300 cycles of charging/discharging. The calculation formula is as follows:
the 300 th cycle capacity retention (%) was (300 th cycle discharge capacity/first cycle discharge capacity) × 100%.
Table 2 results of cell performance test of examples and comparative examples
As can be seen from the results of the electrochemical performance tests of examples 1-10 and comparative example 1 in Table 2, the isocyanate additive of the present invention can improve the electrochemical performance of lithium cobaltate high voltage batteries in different ranges when combined with other additives, wherein the electrochemical performance is improved most remarkably when 1, 6-hexamethylene diisocyanate (compound 1) is added into the electrolyte.
The inventor deduces through literature reading and other related basic experiments that the action mechanism of the substances is mainly that the substances can be oxidized and decomposed on the surface of the anode material to form a passivation film, and the anode material is prevented from being corroded by hydrofluoric acid, so that the dissolution of metal ions (Co) and the collapse of a material structure are avoided.
It will be readily understood by those skilled in the art that the above embodiments may be modified and adapted by persons skilled in the art based on the disclosure and teachings of the above specification, and any modifications, equivalents, improvements and the like made within the spirit and principle of the present invention should be included within the scope of the present invention. Furthermore, although specific terms are employed herein, they are used in a generic and descriptive sense only and not for purposes of limitation.
Claims (10)
1. The non-aqueous electrolyte of the high-voltage lithium cobalt oxide lithium ion battery comprises a non-aqueous organic solvent, an electrolyte lithium salt and an additive, and is characterized in that the additive comprises the following components in percentage by mass in the electrolyte:
0.5 to 1.0 percent of isocyanate additive
0.5 to 20 percent of other additives
2. The non-aqueous electrolyte solution for a high-voltage lithium cobalt oxide lithium ion battery as claimed in claim 1, wherein the isocyanate additive has a structural formula shown in formula (i) or formula (ii):
wherein R, R2，R3It is an alkyl group, a fluoroalkyl group, a phenyl group or an aryl group.
3. The nonaqueous electrolyte solution for a high-voltage lithium cobaltate lithium ion battery according to claim 2, wherein the isocyanate additive is at least one selected from 1, 6-hexamethylene diisocyanate, vinyl isocyanate, isopropyl isocyanate, cyclohexyl isocyanate, p-benzyl isocyanate and ethyl isocyanate.
4. The non-aqueous electrolyte for a high voltage lithium cobalt oxide lithium ion battery as claimed in claim 1, wherein the electrolyte lithium salt is a mixture of lithium hexafluorophosphate, lithium difluorosulfonimide and lithium difluorophosphate.
5. The non-aqueous electrolyte solution for a high-voltage lithium cobalt oxide lithium ion battery as claimed in claim 1, wherein the content of the electrolyte lithium salt in the electrolyte solution is 14.5-17.5% by mass.
6. The non-aqueous electrolyte for a high voltage lithium cobalt oxide lithium ion battery as claimed in claim 1, wherein the other additive is one or more of fluoroethylene carbonate, 1,3, 6-hexanetricarbonitrile, 1, 3-propanesultone, adiponitrile, vinyl sulfate, succinonitrile, 1, 2-bis (cyanoethoxy) ethane.
7. The non-aqueous electrolyte solution for a high-voltage lithium cobalt oxide lithium ion battery according to claim 6, wherein the other additive is a mixture of fluoroethylene carbonate, 1, 3-propane sultone, adiponitrile, and 1, 2-bis (cyanoethoxy) ethane.
8. The nonaqueous electrolyte solution for a high-voltage lithium cobalt oxide lithium ion battery according to claim 1, wherein the nonaqueous organic solvent is a mixture of one or more of cyclic carbonates, chain carbonates, and carboxylates.
9. The non-aqueous electrolyte for a high voltage lithium cobalt oxide lithium ion battery as claimed in claim 8, wherein the non-aqueous organic solvent is a mixture of ethylene carbonate, propylene carbonate, diethyl carbonate, ethyl propionate and propyl propionate.
10. A high voltage lithium cobalt oxide lithium ion battery comprising a cell formed by stacking or winding a positive electrode sheet, a separator and a negative electrode sheet, and the high voltage lithium cobalt oxide lithium ion battery electrolyte according to any one of claims 1 to 9.
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