CN111354978A - High-voltage ternary lithium ion battery electrolyte and high-voltage ternary lithium ion battery - Google Patents
High-voltage ternary lithium ion battery electrolyte and high-voltage ternary lithium ion battery Download PDFInfo
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- CN111354978A CN111354978A CN202010156810.1A CN202010156810A CN111354978A CN 111354978 A CN111354978 A CN 111354978A CN 202010156810 A CN202010156810 A CN 202010156810A CN 111354978 A CN111354978 A CN 111354978A
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- lithium ion
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 60
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 45
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 45
- -1 sulfonate compound Chemical class 0.000 claims abstract description 32
- 229910019142 PO4 Inorganic materials 0.000 claims abstract description 20
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 claims abstract description 20
- 239000010452 phosphate Substances 0.000 claims abstract description 20
- LVTJOONKWUXEFR-FZRMHRINSA-N protoneodioscin Natural products O(C[C@@H](CC[C@]1(O)[C@H](C)[C@@H]2[C@]3(C)[C@H]([C@H]4[C@@H]([C@]5(C)C(=CC4)C[C@@H](O[C@@H]4[C@H](O[C@H]6[C@@H](O)[C@@H](O)[C@@H](O)[C@H](C)O6)[C@@H](O)[C@H](O[C@H]6[C@@H](O)[C@@H](O)[C@@H](O)[C@H](C)O6)[C@H](CO)O4)CC5)CC3)C[C@@H]2O1)C)[C@H]1[C@H](O)[C@H](O)[C@H](O)[C@@H](CO)O1 LVTJOONKWUXEFR-FZRMHRINSA-N 0.000 claims abstract description 20
- 229940126062 Compound A Drugs 0.000 claims abstract description 19
- NLDMNSXOCDLTTB-UHFFFAOYSA-N Heterophylliin A Natural products O1C2COC(=O)C3=CC(O)=C(O)C(O)=C3C3=C(O)C(O)=C(O)C=C3C(=O)OC2C(OC(=O)C=2C=C(O)C(O)=C(O)C=2)C(O)C1OC(=O)C1=CC(O)=C(O)C(O)=C1 NLDMNSXOCDLTTB-UHFFFAOYSA-N 0.000 claims abstract description 19
- 239000000654 additive Substances 0.000 claims abstract description 18
- 230000000996 additive effect Effects 0.000 claims abstract description 16
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims abstract description 15
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 8
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 8
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 8
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims abstract description 4
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims abstract description 4
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims abstract description 4
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 10
- 229910052744 lithium Inorganic materials 0.000 claims description 10
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 9
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 claims description 9
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 6
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 6
- 229910013406 LiN(SO2CF3)2 Inorganic materials 0.000 claims description 6
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical class [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 claims description 6
- 229910045601 alloy Inorganic materials 0.000 claims description 6
- 239000000956 alloy Substances 0.000 claims description 6
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 6
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 6
- 229910052723 transition metal Inorganic materials 0.000 claims description 6
- 239000011149 active material Substances 0.000 claims description 5
- 229910021383 artificial graphite Inorganic materials 0.000 claims description 4
- 229910052751 metal Inorganic materials 0.000 claims description 4
- 239000002184 metal Substances 0.000 claims description 4
- GWAOOGWHPITOEY-UHFFFAOYSA-N 1,5,2,4-dioxadithiane 2,2,4,4-tetraoxide Chemical compound O=S1(=O)CS(=O)(=O)OCO1 GWAOOGWHPITOEY-UHFFFAOYSA-N 0.000 claims description 3
- 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 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 3
- 229910013089 LiBF3 Inorganic materials 0.000 claims description 3
- 229910013188 LiBOB Inorganic materials 0.000 claims description 3
- 229910000552 LiCF3SO3 Inorganic materials 0.000 claims description 3
- 229910010941 LiFSI Inorganic materials 0.000 claims description 3
- 229910013385 LiN(SO2C2F5)2 Inorganic materials 0.000 claims description 3
- 229910013884 LiPF3 Inorganic materials 0.000 claims description 3
- 229910001290 LiPF6 Inorganic materials 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- OBNDGIHQAIXEAO-UHFFFAOYSA-N [O].[Si] Chemical compound [O].[Si] OBNDGIHQAIXEAO-UHFFFAOYSA-N 0.000 claims description 3
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 claims description 3
- 125000004432 carbon atom Chemical group C* 0.000 claims description 3
- PYMZYVXDCJXPAM-UHFFFAOYSA-N ethane-1,2-diol;propanenitrile Chemical compound CCC#N.CCC#N.OCCO PYMZYVXDCJXPAM-UHFFFAOYSA-N 0.000 claims description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 3
- 229910021385 hard carbon Inorganic materials 0.000 claims description 3
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 claims description 3
- 229910001547 lithium hexafluoroantimonate(V) Inorganic materials 0.000 claims description 3
- 229910001947 lithium oxide Inorganic materials 0.000 claims description 3
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 3
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 3
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 3
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-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
- 239000002905 metal composite material Substances 0.000 claims description 3
- 229910044991 metal oxide Inorganic materials 0.000 claims description 3
- 150000004706 metal oxides Chemical class 0.000 claims description 3
- 229910021382 natural graphite Inorganic materials 0.000 claims description 3
- MHYFEEDKONKGEB-UHFFFAOYSA-N oxathiane 2,2-dioxide Chemical compound O=S1(=O)CCCCO1 MHYFEEDKONKGEB-UHFFFAOYSA-N 0.000 claims description 3
- 229910021384 soft carbon Inorganic materials 0.000 claims description 3
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 claims description 3
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-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
- 125000001153 fluoro group Chemical group F* 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
- 125000001183 hydrocarbyl group Chemical group 0.000 claims 8
- 230000002195 synergetic effect Effects 0.000 abstract description 3
- 230000000052 comparative effect Effects 0.000 description 21
- 150000001875 compounds Chemical class 0.000 description 16
- 150000002430 hydrocarbons Chemical group 0.000 description 14
- 230000006872 improvement Effects 0.000 description 11
- 230000015572 biosynthetic process Effects 0.000 description 7
- 238000007600 charging Methods 0.000 description 7
- 230000002829 reductive effect Effects 0.000 description 7
- 230000014759 maintenance of location Effects 0.000 description 6
- 238000012360 testing method Methods 0.000 description 6
- 238000011056 performance test Methods 0.000 description 5
- 239000007774 positive electrode material Substances 0.000 description 5
- 238000003860 storage Methods 0.000 description 5
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 238000002360 preparation method Methods 0.000 description 4
- 238000003466 welding Methods 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 3
- 238000007599 discharging Methods 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 238000002161 passivation Methods 0.000 description 3
- 150000003624 transition metals Chemical class 0.000 description 3
- 239000006245 Carbon black Super-P Substances 0.000 description 2
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- 229910052782 aluminium Inorganic materials 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
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 230000002542 deteriorative effect Effects 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000011267 electrode slurry Substances 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 238000005096 rolling process Methods 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 238000001291 vacuum drying Methods 0.000 description 2
- ZPFAVCIQZKRBGF-UHFFFAOYSA-N 1,3,2-dioxathiolane 2,2-dioxide Chemical compound O=S1(=O)OCCO1 ZPFAVCIQZKRBGF-UHFFFAOYSA-N 0.000 description 1
- IFDLFCDWOFLKEB-UHFFFAOYSA-N 2-methylbutylbenzene Chemical compound CCC(C)CC1=CC=CC=C1 IFDLFCDWOFLKEB-UHFFFAOYSA-N 0.000 description 1
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910012258 LiPO Inorganic materials 0.000 description 1
- 230000010718 Oxidation Activity Effects 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
- 239000013543 active substance Substances 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 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
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000010280 constant potential charging Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 125000003709 fluoroalkyl group Chemical group 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- VLKZOEOYAKHREP-UHFFFAOYSA-N hexane Substances CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000006864 oxidative decomposition reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 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
- 239000002985 plastic film Substances 0.000 description 1
- 229920006255 plastic film Polymers 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 239000002153 silicon-carbon composite material Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910001428 transition metal ion Inorganic materials 0.000 description 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 1
- 238000009461 vacuum packaging Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 238000004804 winding 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
- H01M10/052—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
- H01M10/05—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
- H01M10/42—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
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- 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 belongs to the technical field of lithium ion batteries, and particularly relates to a high-voltage ternary lithium ion battery electrolyte which comprises a lithium salt, a non-aqueous organic solvent and an additive, wherein the additive contains vinylene carbonate, 1, 3-propane sultone and fluoroethylene carbonate, and also comprises a combination of a phosphate compound A, a sulfonate compound B and a sulfite compound C. Compared with the prior art, the electrolyte provided by the invention can improve the high-temperature performance of the lithium ion battery under high voltage through the synergistic effect of the compound A, B, C, and also greatly improves the cycle performance and low-temperature performance of the battery. In addition, the invention also provides a high-voltage ternary lithium ion battery using the electrolyte.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a high-voltage ternary lithium ion battery electrolyte and a high-voltage ternary lithium ion battery.
Background
With the continuous improvement of the energy density requirement of the lithium ion battery, the charge cut-off voltage of the ternary lithium ion battery is also continuously improved, and the defects of reduced full-charge high-temperature storage performance, quick high-temperature cycle life decay, low-temperature discharge lithium precipitation and the like generally exist in the high-voltage ternary lithium ion battery with the voltage of 4.35V and above in the current market compared with the ternary lithium ion battery with the voltage of below 4.35V.
The charge cut-off voltage of the ternary battery is increased from 4.35V to 4.40V or more, and the energy density of the ternary battery is remarkably improved. At the same time, however, the performance of the battery, particularly the high-temperature cycle and high-temperature storage performance of the battery, is significantly reduced. At present, the modification research on the NCM ternary material continuously increases the content of nickel, so that the lattice stability of the ternary material is gradually reduced, and therefore, the ternary material is easy to collapse in structure under the high-temperature and high-pressure environment and is accompanied with the release of oxygen and the dissolution of transition metal. The reasons for these problems are mainly:
1) the electrolyte is oxidized and decomposed on the surface of the positive electrode material. Under high voltage, the oxidation activity of the anode active material is higher, and the reaction between the anode active material and the electrolyte is further accelerated under high temperature conditions, so that the oxidative decomposition products of the electrolyte are continuously deposited on the surface of the anode, and the internal resistance and the thickness of the battery are continuously increased.
2) And dissolving out and reducing metal ions in the crystal lattice of the positive electrode material. In one aspect, LiPF in an electrolyte at high temperatures6HF generated by decomposition is extremely easy to corrode the positive active material, so that metal ions are dissolved out; on the other hand, under high voltage, the transition metal oxide of the positive active material is easily reduced and dissolved out, and the transition metal ions are reduced into a metal simple substance on the surface of the negative electrode after passing through the SEI film, so that the impedance of the negative electrode is continuously increased, and the battery performance is deteriorated.
Therefore, it is necessary to develop a new electrolyte to overcome the above problems, and further to improve the voltage resistance, long cycle life, and safety of the battery.
Disclosure of Invention
One of the objects of the present invention is: aiming at the defects of the prior art, the electrolyte of the high-voltage ternary lithium ion battery is provided, and the high-temperature performance of the ternary lithium ion battery under high voltage is improved, and meanwhile, the cycle performance and the low-temperature performance of the ternary lithium ion battery are greatly improved.
In order to achieve the purpose, the invention adopts the following technical scheme:
the high-voltage ternary lithium ion battery electrolyte is characterized in that: the additive comprises a lithium salt, a non-aqueous organic solvent and an additive, wherein the additive comprises vinylene carbonate, 1, 3-propane sultone and fluoroethylene carbonate, and also comprises at least two of a phosphate compound A, a sulfonate compound B and a sulfite compound C.
As an improvement of the high-voltage ternary lithium ion battery electrolyte, the structural formula of the phosphate compound A is shown as the formula I:
wherein R is1～R3Each independently selected from a C1-6 hydrocarbon group, a fluorinated hydrocarbon group, and a silane group.
As an improvement of the high-voltage ternary lithium ion battery electrolyte, the structural formula of the sulfonate compound B is shown as a formula II:
wherein R is4Selected from C1-6 hydrocarbon group, fluoro hydrocarbon group or silane group, R5Selected from a C1-6 hydrocarbon group or a fluorinated hydrocarbon group.
As an improvement of the high-voltage ternary lithium ion battery electrolyte, the structural formula of the sulfite compound C is shown as the formula III:
wherein R is6Selected from a hydrocarbon group having 1 to 3 carbon atoms, a fluorinated hydrocarbon group or
Preferably, the phosphate compound a is at least one of the following compounds:
preferably, the sulfonate compound B is at least one of the following compounds:
preferably, the sulfite compound C is at least one of the following compounds:
more preferably, the phosphate ester compound A is
The sulfonate compound B is
The sulfite compound C is
As an improvement of the high-voltage ternary lithium ion battery electrolyte, the mass of the phosphate compound A accounts for 0.1-5.0% of the total mass of the electrolyte, the mass of the sulfonate compound B accounts for 0.1-15.0% of the total mass of the electrolyte, and the mass of the sulfite compound C accounts for 0.1-10.0% of the total mass of the electrolyte. Preferably, the addition of the three compounds causes too thick film formation and too large impedance, thereby deteriorating the battery performance; and if the addition amount is too small, the effect is not obvious. Therefore, the mass of the phosphate compound A is preferably 0.1-2.0% of the total mass of the electrolyte, the mass of the sulfonate compound B is preferably 0.1-5.0% of the total mass of the electrolyte, and the mass of the sulfite compound C is preferably 0.1-3.0% of the total mass of the electrolyte.
As an improvement of the electrolyte of the high-voltage ternary lithium ion battery, the non-aqueous organic solvent comprises at least one of ethylene carbonate, ethyl methyl carbonate, diethyl carbonate, propylene carbonate, ethyl propionate and propyl propionate.
As an improvement of the high-voltage ternary lithium ion battery electrolyte, the additive further comprises at least one of lithium difluorophosphate, 1, 4-butane sultone, 1, 3-propylene sultone, ethylene carbonate, ethylene sulfate, methylene methane disulfonate, succinonitrile, adiponitrile, ethylene glycol dipropionitrile ether and 1,3, 6-hexane tricarbonitrile.
As an improvement of the high-voltage ternary lithium ion battery electrolyte, the lithium salt is LiPF6、LiBF4、LiClO4、LiFSI、LiTFSI、LiBOB、LiDFOB、LiFAP、LiSbF6、LiCF3SO3、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiN(SO2CF3)2、LiN(SO2C4F9)2、LiC(SO2CF3)3、LiPF3(C3F7)3、LiB(CF3)4And LiBF3(C2F5) At least one of (1).
The second purpose of the invention is: the high-voltage ternary lithium ion battery comprises an anode, a cathode, a diaphragm and electrolyte, wherein the electrolyte is the high-voltage ternary lithium ion battery electrolyte described in any section in the specification, and the charge cut-off voltage of the high-voltage ternary lithium ion battery is 4.4-4.6V.
As an improvement of the high-voltage ternary lithium ion battery, an active substance of the positive electrode is a lithium transition metal composite oxide; the active material of the negative electrode is at least one of soft carbon, hard carbon, artificial graphite, natural graphite, silicon-oxygen compound, silicon-carbon compound, lithium titanate, metal or alloy capable of forming an alloy with lithium and metal oxide capable of inserting/extracting lithium.
Compared with the prior art, the invention at least has the following beneficial effects:
1) the phosphate ester compound A is added into the electrolyte, and can form a film on the surface of the positive electrode of the battery in the battery formation stage, so that the continuous decomposition of the electrolyte on the surface of the electrode is prevented, and the high-temperature storage performance and the cycle performance of the battery are improved.
2) The electrolyte is added with the sulfonate compound B, and the sulfonate compound B is subjected to reductive decomposition in preference to a solvent in the battery formation process to form an SEI film on a negative electrode. The SEI film has low impedance, and the low-temperature discharge performance and the normal-temperature cycle performance of the battery are greatly improved.
3) The sulfite compound C is added into the electrolyte, so that a stable passivation film can be formed on the positive electrode and the negative electrode of the battery, the passivation film has low impedance performance, and the low-temperature performance of the lithium ion battery can be improved; and the film has the advantages of thin thickness, good compactness and high stability, can protect the positive and negative electrode interfaces, and improves the stability of the electrolyte, thereby improving the high-temperature storage and high-temperature cycle performance of the battery.
4) Although the film-forming impedance of the phosphate compound A is too large to affect the normal-temperature cycle and low-temperature performance, the oxidation potential of the sulfonate compound B is too low to cause poor high-temperature performance, and the improvement of the high-temperature storage and high-temperature cycle performance by the sulfite compound C is relatively limited, the phosphate compound A, the sulfonate compound B and the sulfite compound C are simultaneously added into the electrolyte, and the phosphate compound A, the sulfonate compound B and the sulfite compound C form a passivation film with strong oxidizing property and low impedance through the synergistic action of the positive electrode and the negative electrode, so that the comprehensive performance of the battery is greatly improved.
Detailed Description
A high-voltage ternary lithium ion battery with a charge cut-off voltage of 4.4-4.6V comprises a positive electrode, a negative electrode, a diaphragm and electrolyte.
The active material of the positive electrode is a lithium transition metal composite oxide, including but not limited to lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminum oxide, compounds of the foregoing oxides with other transition metals or non-transition metals added, or combinations thereof.
The active material of the negative electrode is at least one of soft carbon, hard carbon, artificial graphite, natural graphite, silicon-oxygen compound, silicon-carbon composite, lithium titanate, metal or alloy capable of forming an alloy with lithium, and metal oxide capable of inserting/extracting lithium.
The high-voltage ternary lithium ion battery electrolyte comprises a lithium salt, a nonaqueous organic solvent and an additive, wherein the additive comprises the lithium salt, the nonaqueous organic solvent and the additive, and the additive comprises at least two of a phosphate compound A, a sulfonate compound B and a sulfite compound C besides vinylene carbonate, 1, 3-propane sultone and fluoroethylene carbonate.
The structural formula of the phosphate compound A is shown as the formula I:
wherein R is1～R3Each independently selected from a C1-6 hydrocarbon group, a fluorinated hydrocarbon group, a silane group, etc.;
the structural formula of the sulfonate compound B is shown as the formula II:
wherein R is4Selected from C1-6 hydrocarbon group, fluorinated hydrocarbon group, silane group, etc5Selected from alkyl or fluoro alkyl with 1-6 carbon atoms;
the structural formula of the sulfite compound C is shown as the formula III:
wherein R is6Selected from a C1-3 hydrocarbon group or a fluorinated hydrocarbon group,
And the like.
Preferably, the phosphate compound a is at least one of the following compounds:
preferably, the sulfonate compound B is at least one of the following compounds:
preferably, the sulfite compound C is at least one of the following compounds:
more preferably, the phosphate ester compound A is
The sulfonate compound B is
The sulfite compound C is
Preferably, the mass of the phosphate compound A accounts for 0.1-5.0% of the total mass of the electrolyte, the mass of the sulfonate compound B accounts for 0.1-15.0% of the total mass of the electrolyte, and the mass of the sulfite compound C accounts for 0.1-10.0% of the total mass of the electrolyte. Further preferably, the addition of the three compounds causes too thick film formation and too large impedance, thereby deteriorating the battery performance; and if the addition amount is too small, the effect is not obvious. Therefore, the mass of the phosphate compound A is preferably 0.1-2.0% of the total mass of the electrolyte, the mass of the sulfonate compound B is preferably 0.1-5.0% of the total mass of the electrolyte, and the mass of the sulfite compound C is preferably 0.1-3.0% of the total mass of the electrolyte.
Preferably, the non-aqueous organic solvent includes at least one of ethylene carbonate, ethyl methyl carbonate, diethyl carbonate, propylene carbonate, ethyl propionate, and propyl propionate.
Preferably, the additive further comprises at least one of lithium difluorophosphate, 1, 4-butane sultone, 1, 3-propene sultone, ethylene carbonate, vinyl sulfate, methylene methanedisulfonate, succinonitrile, adiponitrile, ethylene glycol dipropionitrile ether, and 1,3, 6-hexane trinitrile.
Preferably, the lithium salt is LiPF6、LiBF4、LiClO4、LiFSI、LiTFSI、LiBOB、LiDFOB、LiFAP、LiSbF6、LiCF3SO3、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiN(SO2CF3)2、LiN(SO2C4F9)2、LiC(SO2CF3)3、LiPF3(C3F7)3、LiB(CF3)4And LiBF3(C2F5) At least one of (1).
In order to make the technical solution and advantages of the present invention clearer, the present invention is described in further detail with reference to the following embodiments, but the embodiments of the present invention are not limited thereto.
In the following comparative examples and examples, the compounds a, b, c used have the following structural formula:
comparative example 1
1) Preparation of positive plate
The positive electrode active material NCM523, the conductive carbon black Super-P, and the binder polyvinylidene fluoride (PVDF) were mixed in a mass ratio of 93:4:3, and then dispersed in N-methyl-2-pyrrolidone (NMP) to obtain a positive electrode slurry. And uniformly coating the slurry on two sides of the aluminum foil, drying, rolling and vacuum drying, and welding an aluminum outgoing line by using an ultrasonic welding machine to obtain the positive plate, wherein the thickness of the pole piece is 120-150 mu m.
2) Preparation of negative plate
Mixing artificial graphite serving as a negative electrode active material, conductive carbon black Super-P, Styrene Butadiene Rubber (SBR) serving as a binder and carboxymethyl cellulose (CMC) according to a mass ratio of 94:1:2.5:2.5, and dispersing the materials in ionized water to obtain negative electrode slurry. Coating the slurry on two sides of the copper foil, drying, rolling and vacuum drying, and welding a nickel outgoing line by using an ultrasonic welding machine to obtain the negative plate, wherein the thickness of the pole piece is 120-150 mu m.
3) Preparation of the electrolyte
Mixing Ethylene Carbonate (EC), diethyl carbonate (DEC), Propylene Carbonate (PC) and the mixture according to the mass ratio EC: DEC: PC: 2:6:2, and adding 0.5 wt% of VC, 4.0 wt% of FEC, 2 wt% of PS, 0.5 wt% of wtADN and 1 wt% of LiPO respectively2F2Then, 14.0 wt% of lithium hexafluorophosphate (LiPF) was added in mass fraction6) Fully mixing and dissolving for later use.
4) Preparation of the Battery
Placing an isolating membrane with the thickness of 16 mu m between the positive plate and the negative plate, then winding a sandwich structure consisting of the positive plate, the negative plate and the diaphragm, flattening the wound body, then placing the flattened wound body into an aluminum-plastic film packaging bag, and baking the flattened wound body in vacuum at 80 ℃ for 48 hours to obtain a battery cell to be injected with liquid; respectively injecting the prepared electrolyte into a battery cell in a glove box with the dew point controlled below-40 ℃, carrying out vacuum packaging, standing for 24h, and then carrying out conventional formation and capacity grading according to the following steps: charging at 0.05C for 180min, charging at 0.2C to 4.0V, and vacuum sealing twice; further charging to 4.6V at a constant current of 0.2C, standing at normal temperature for 24h, and discharging to 3.0V at a constant current of 0.2C; and finally, charging the mixture to 4.6V at a constant current of 1C for standing.
Comparative examples 2 to 10
In comparative examples 2 to 10, the components and contents of the additives are the same as those in comparative example 1, and the description thereof is omitted. Specifically, the results are shown in Table 1.
Examples 1 to 4
In examples 1 to 4, the components and contents of the additives were the same as those in comparative example 1, and the description thereof is omitted. Specifically, the results are shown in Table 1.
Performance testing
The batteries prepared in comparative examples 1 to 10 and examples 1 to 4 were subjected to a performance test.
1) EIS Performance test
Taking the battery cell after the capacity grading of comparative examples 1-10 and examples 1-4 to perform EIS test, wherein the test conditions are as follows: the frequency range is 100 kHz-0.01 Hz, and the amplitude is 10 mV; the tested data were subjected to circuit fitting to obtain SEI impedance, the results of which are shown in table 1.
2) High temperature cycle performance test
The batteries prepared in comparative examples 1 to 10 and examples 1 to 4 were placed in an oven at a constant temperature of 45 ℃, and were charged to 4.6V at a constant current of 1C and then the constant voltage charging current was decreased to 0.02C, and then discharged to 3.0V at a constant current of 1C, and the cycle was repeated for 100 weeks, and the discharge capacity per week was recorded, and the capacity retention rate at high temperature cycle was calculated according to the following formula: the n-week capacity retention rate is 100% of the n-week discharge capacity/1-week discharge capacity.
3) Test of ordinary temperature cycle Performance
Taking the batteries prepared in comparative examples 1 to 10 and examples 1 to 4, charging the batteries to 4.6V at room temperature by a current of 1C at a constant current, then charging the batteries at a constant voltage until the current is reduced to 0.1C, then discharging the batteries to 3.0V at a current of 1C at a constant current, circulating the process for 100 weeks, recording the discharge capacity of each week, and calculating the capacity retention rate of the batteries in normal-temperature circulation according to the following formula: capacity retention rate at m weeks was 100% of discharge capacity at m weeks/discharge capacity at 1 week.
4) Low temperature discharge performance test
At 25 ℃, the batteries formed in comparative examples 1 to 10 and examples 1 to 4 were charged to 4.6V with a constant current and a constant voltage of 1C, and then discharged to 3.0V with a constant current of 1C, and the discharge capacity C1 was recorded; and then charging to 4.6V at constant current and constant voltage of 1C, standing for 4h in an environment at 0 ℃, discharging to 3.0V at constant current of 0.2C, and recording the discharge capacity C2. Wherein the low-temperature discharge efficiency value at 0 ℃ is C2/C1 x 100%.
The specific results of the above performance tests are shown in tables 1 and 2.
TABLE 1 EIS test results
TABLE 2 test results of cycle capacity retention and low-temperature discharge retention
| Examples of the experiments | Additive agent | 100cls@45℃ | 100cls@25℃ | 0.2C@0℃ |
| Comparative example 1 | / | 53.12 | 57.36 | 83.54 |
| Comparative example 2 | 0.2wt％a | 55.35 | 59.78 | 80.25 |
| Comparative example 3 | 1wt％a | 58.82 | 61.15 | 76.38 |
| Comparative example 4 | 2wt％a | 56.25 | 60.52 | 73.15 |
| Comparative example 5 | 0.2wt％b | 54.36 | 59.21 | 84.39 |
| Comparative example 6 | 1wt％b | 52.24 | 62.39 | 86.55 |
| Comparative example 7 | 5wt％b | 50.03 | 61.11 | 80.53 |
| Comparative example 8 | 0.2wt％c | 57.38 | 60.32 | 84.22 |
| Comparative example 9 | 1wt％c | 63.84 | 64.83 | 85.92 |
| Comparative example 10 | 3wt％c | 61.75 | 62.07 | 79.65 |
| Example 1 | 1wt％a+1wt％b | 68.56 | 72.58 | 83.55 |
| Example 2 | 1wt％a+1wt％c | 70.61 | 79.56 | 81.12 |
| Example 3 | 1wt％b+1wt％c | 64.58 | 81.31 | 88.23 |
| Example 4 | 1wt％a+1wt％b+1wt％c | 77.61 | 84.54 | 91.15 |
As can be seen from the data in tables 1 and 2:
1) by adding the three compounds a, b, c alone and in combination, it was found that the addition of compounds b, c at high voltage reduces the film formation resistance, and the addition of compound a increases the film formation resistance. By the synergistic effect, the combination of the three compounds can obviously reduce the film forming resistance;
2) when the compounds a, b and c with different contents are respectively added into the electrolyte, the comprehensive performance is better than other content ratio when the content is 1 wt%;
3) the combination performance of the three compounds a, b and c is obviously improved, wherein the combination of 1 wt% of a +1 wt% of b +1 wt% of c has the best combination performance.
Variations and modifications to the above-described embodiments may also occur to those skilled in the art, which fall within the scope of the invention as disclosed and taught herein. Therefore, the present invention is not limited to the above-mentioned embodiments, and any obvious improvement, replacement or modification made by those skilled in the art based on the present invention is within the protection 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 high-voltage ternary lithium ion battery electrolyte is characterized in that: the additive comprises a lithium salt, a non-aqueous organic solvent and an additive, wherein the additive comprises vinylene carbonate, 1, 3-propane sultone and fluoroethylene carbonate, and also comprises at least two of a phosphate compound A, a sulfonate compound B and a sulfite compound C.
2. The high-voltage ternary lithium ion battery electrolyte according to claim 1, wherein the phosphate compound A has a structural formula shown in formula I:
wherein R is1～R3Each independently selected from a C1-6 hydrocarbon group, a fluorinated hydrocarbon group, and a silane group.
3. The high-voltage ternary lithium ion battery electrolyte of claim 1, wherein the structural formula of the sulfonate compound B is shown as formula II:
wherein R is4Selected from C1-6 hydrocarbon group, fluoro hydrocarbon group or silane group, R5Selected from a C1-6 hydrocarbon group or a fluorinated hydrocarbon group.
4. The high voltage ternary lithium ion battery electrolyte of claim 1, wherein: the structural formula of the sulfite compound C is shown as the formula III:
wherein R is6Selected from a hydrocarbon group having 1 to 3 carbon atoms, a fluorinated hydrocarbon group or
5. The high voltage ternary lithium ion battery electrolyte of claim 1, wherein: the mass of the phosphate compound A accounts for 0.1-5.0% of the total mass of the electrolyte, the mass of the sulfonate compound B accounts for 0.1-15.0% of the total mass of the electrolyte, and the mass of the sulfite compound C accounts for 0.1-10.0% of the total mass of the electrolyte.
6. The high voltage ternary lithium ion battery electrolyte of claim 1, wherein: the non-aqueous organic solvent includes at least one of ethylene carbonate, ethyl methyl carbonate, diethyl carbonate, propylene carbonate, ethyl propionate, and propyl propionate.
7. The high voltage ternary lithium ion battery electrolyte of claim 1, wherein: the additive also comprises at least one of lithium difluorophosphate, 1, 4-butane sultone, 1, 3-propylene sultone, ethylene carbonate, vinyl sulfate, methylene methane disulfonate, succinonitrile, adiponitrile, ethylene glycol dipropionitrile ether and 1,3, 6-hexane tricarbonitrile.
8. The high voltage ternary lithium ion battery electrolyte of claim 1, wherein: the lithium salt is LiPF6、LiBF4、LiClO4、LiFSI、LiTFSI、LiBOB、LiDFOB、LiFAP、LiSbF6、LiCF3SO3、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiN(SO2CF3)2、LiN(SO2C4F9)2、LiC(SO2CF3)3、LiPF3(C3F7)3、LiB(CF3)4And LiBF3(C2F5) At least one of (1).
9. The utility model provides a high voltage ternary lithium ion battery, includes positive pole, negative pole, diaphragm and electrolyte, its characterized in that: the electrolyte is the electrolyte of the high-voltage ternary lithium ion battery as claimed in any one of claims 1 to 8, and the charge cut-off voltage of the high-voltage ternary lithium ion battery is 4.4V-4.6V.
10. The high voltage ternary lithium ion battery of claim 9, wherein: the active material of the positive electrode is a lithium transition metal composite oxide; the active material of the negative electrode is at least one of soft carbon, hard carbon, artificial graphite, natural graphite, silicon-oxygen compound, silicon-carbon compound, lithium titanate, metal or alloy capable of forming an alloy with lithium and metal oxide capable of inserting/extracting lithium.
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