CN116646597A - Electrolyte and battery comprising same - Google Patents
Electrolyte and battery comprising same Download PDFInfo
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- CN116646597A CN116646597A CN202310497335.8A CN202310497335A CN116646597A CN 116646597 A CN116646597 A CN 116646597A CN 202310497335 A CN202310497335 A CN 202310497335A CN 116646597 A CN116646597 A CN 116646597A
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- electrolyte
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 66
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 26
- 239000002904 solvent Substances 0.000 claims abstract description 26
- -1 alkenyl siloxane compounds Chemical class 0.000 claims abstract description 14
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims abstract description 9
- 239000000654 additive Substances 0.000 claims description 27
- 230000000996 additive effect Effects 0.000 claims description 24
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 22
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 12
- 125000000217 alkyl group Chemical group 0.000 claims description 10
- 239000003960 organic solvent Substances 0.000 claims description 7
- 125000003342 alkenyl group Chemical group 0.000 claims description 6
- 125000003118 aryl group Chemical group 0.000 claims description 5
- 150000001875 compounds Chemical class 0.000 claims description 5
- 125000001424 substituent group Chemical group 0.000 claims description 5
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 4
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 4
- 229910052700 potassium Inorganic materials 0.000 claims description 4
- 239000011591 potassium Substances 0.000 claims description 4
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 3
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 claims description 3
- 150000003839 salts Chemical class 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 2
- QUGUFLJIAFISSW-UHFFFAOYSA-N 1,4-difluorobenzene Chemical compound FC1=CC=C(F)C=C1 QUGUFLJIAFISSW-UHFFFAOYSA-N 0.000 claims description 2
- 229920001774 Perfluoroether Polymers 0.000 claims description 2
- 150000004649 carbonic acid derivatives Chemical class 0.000 claims description 2
- 150000007942 carboxylates Chemical class 0.000 claims description 2
- RBBXSUBZFUWCAV-UHFFFAOYSA-N ethenyl hydrogen sulfite Chemical compound OS(=O)OC=C RBBXSUBZFUWCAV-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
- GZKHDVAKKLTJPO-UHFFFAOYSA-N ethyl 2,2-difluoroacetate Chemical group CCOC(=O)C(F)F GZKHDVAKKLTJPO-UHFFFAOYSA-N 0.000 claims description 2
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 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
- PYLWMHQQBFSUBP-UHFFFAOYSA-N monofluorobenzene Chemical compound FC1=CC=CC=C1 PYLWMHQQBFSUBP-UHFFFAOYSA-N 0.000 claims description 2
- YZYKZHPNRDIPFA-UHFFFAOYSA-N tris(trimethylsilyl) borate Chemical compound C[Si](C)(C)OB(O[Si](C)(C)C)O[Si](C)(C)C YZYKZHPNRDIPFA-UHFFFAOYSA-N 0.000 claims description 2
- VMZOBROUFBEGAR-UHFFFAOYSA-N tris(trimethylsilyl) phosphite Chemical compound C[Si](C)(C)OP(O[Si](C)(C)C)O[Si](C)(C)C VMZOBROUFBEGAR-UHFFFAOYSA-N 0.000 claims description 2
- 239000002131 composite material Substances 0.000 abstract description 7
- 230000001681 protective effect Effects 0.000 abstract description 4
- 238000007086 side reaction Methods 0.000 abstract description 4
- 230000003647 oxidation Effects 0.000 abstract description 3
- 238000007254 oxidation reaction Methods 0.000 abstract description 3
- 230000035939 shock Effects 0.000 abstract description 3
- 125000001153 fluoro group Chemical group F* 0.000 abstract description 2
- 150000002500 ions Chemical class 0.000 abstract 1
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 17
- 229910001416 lithium ion Inorganic materials 0.000 description 17
- 239000011230 binding agent Substances 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 10
- 239000006258 conductive agent Substances 0.000 description 10
- 239000007774 positive electrode material Substances 0.000 description 9
- 229910052782 aluminium Inorganic materials 0.000 description 7
- 238000002360 preparation method Methods 0.000 description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 6
- 239000007773 negative electrode material Substances 0.000 description 6
- 238000002474 experimental method Methods 0.000 description 5
- 239000011888 foil Substances 0.000 description 5
- 150000003949 imides Chemical class 0.000 description 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- 239000001768 carboxy methyl cellulose Substances 0.000 description 3
- 238000007599 discharging Methods 0.000 description 3
- 230000014759 maintenance of location Effects 0.000 description 3
- 238000006467 substitution reaction Methods 0.000 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 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 2
- SSBFISCARUPWGN-UHFFFAOYSA-N [Li].C(C(=O)F)(=O)F Chemical compound [Li].C(C(=O)F)(=O)F SSBFISCARUPWGN-UHFFFAOYSA-N 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
- 239000006183 anode active material Substances 0.000 description 2
- 239000006256 anode slurry Substances 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 238000007600 charging Methods 0.000 description 2
- 238000010280 constant potential charging Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 238000005096 rolling process Methods 0.000 description 2
- 239000002109 single walled nanotube Substances 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 2
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 2
- 238000007614 solvation Methods 0.000 description 2
- 239000010959 steel Substances 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 229920003048 styrene butadiene rubber Polymers 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- PBIMIGNDTBRRPI-UHFFFAOYSA-N trifluoro borate Chemical compound FOB(OF)OF PBIMIGNDTBRRPI-UHFFFAOYSA-N 0.000 description 2
- 125000000882 C2-C6 alkenyl group Chemical group 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 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
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 1
- 229910012820 LiCoO Inorganic materials 0.000 description 1
- 229910013872 LiPF Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000002174 Styrene-butadiene Substances 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- ZJPPTKRSFKBZMD-UHFFFAOYSA-N [Li].FS(=N)F Chemical compound [Li].FS(=N)F ZJPPTKRSFKBZMD-UHFFFAOYSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 229910021383 artificial graphite 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
- MTAZNLWOLGHBHU-UHFFFAOYSA-N butadiene-styrene rubber Chemical compound C=CC=C.C=CC1=CC=CC=C1 MTAZNLWOLGHBHU-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- 125000000524 functional group Chemical group 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- 239000003273 ketjen black Substances 0.000 description 1
- 229920000126 latex Polymers 0.000 description 1
- 239000004816 latex Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910003002 lithium salt Inorganic materials 0.000 description 1
- 159000000002 lithium salts Chemical class 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 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
- 230000035515 penetration Effects 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 229920005569 poly(vinylidene fluoride-co-hexafluoropropylene) Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 229940090181 propyl acetate Drugs 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- 239000011115 styrene butadiene Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 238000009461 vacuum packaging Methods 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-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
- H01M10/056—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
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0569—Liquid materials characterised by the solvents
-
- 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
- H01M10/058—Construction or manufacture
-
- 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
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
-
- 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)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
Abstract
The invention provides an electrolyte and a battery comprising the same, and the invention adopts a fluoro solvent and the combination of alkenyl siloxane compounds, lithium difluoro oxalato borate and lithium bis (trifluoromethyl) sulfonyl imide; the three can act together, the composite interface protective film generated on the surfaces of the positive electrode and the negative electrode is firm and low in impedance, side reactions between the electrode and the electrolyte are effectively inhibited, the electrolyte has the characteristic of high ion conductivity, meanwhile, the high-voltage stability of the electrolyte can be further improved by matching with a fluorinated solvent with better oxidation resistance, the safety performance (the thermal shock performance, the overcharging performance and the needling performance can be simultaneously considered) of the battery is improved, and meanwhile, the high-temperature cycle performance and the low-temperature performance of the battery under high voltage are also improved.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to high-voltage-resistant high-safety electrolyte and a battery comprising the same.
Background
Since commercialization, the lithium ion battery is widely used in the fields of digital, energy storage, power, military aerospace, communication equipment and the like due to high specific energy and good cycle performance. With the wide application of lithium ion batteries, the use environment and the demands of consumers on the lithium ion batteries are continuously improved, the lithium ion batteries are required to be advanced towards higher energy density, and meanwhile, the long cycle performance and the safety performance of the lithium ion batteries are required to be maintained, and the energy density is further improved, so that the battery voltage is required to be improved or the battery capacity is required to be improved.
At present, the voltage of a commercial lithium ion battery is basically below 4.48V, and when the voltage further reaches above 4.48V, the traditional commercial carbonate electrolyte is difficult to withstand such high voltage, the side reaction of a positive electrode is obviously aggravated, and the improvement of the enough good long-cycle stability can not be realized by an additive strategy alone. In addition to significant cycle degradation, battery safety, stored gas production, and cycle expansion are also significantly exacerbated. Therefore, there is an urgent need to develop a high-voltage electrolyte for lithium ion batteries that can perform safety protection without affecting the high-temperature performance of the batteries.
Disclosure of Invention
The invention aims to solve the problems of reduced service life, poor safety performance and the like of the traditional lithium ion battery caused by aggravated side reaction between an electrode and electrolyte at high voltage, and provides the electrolyte and the battery comprising the electrolyte.
In order to achieve the above purpose, the technical scheme adopted by the invention is as follows:
an electrolyte comprising an organic solvent, an additive, and an electrolyte salt; the additive comprises a first additive selected from the group consisting of alkenylsiloxanes, lithium difluorooxalato borate, and lithium bistrifluoromethylsulfonimide;
the organic solvent comprises a fluorinated solvent; the fluorinated solvent comprises a first fluorinated solvent and a second fluorinated solvent; the first fluorinated solvent is selected from ethyl 2, 2-difluoroacetate; the second fluorinated solvent includes at least one of a fluorinated carbonate, a fluorinated carboxylate, a fluoroether, and a fluorobenzene.
According to an embodiment of the present invention, the alkenylsiloxane compound is a siloxane compound containing an alkenyl group.
According to an embodiment of the present invention, the alkenylsiloxane compound has a structural formula shown in formula I:
in the formula I, R 1 、R 2 、R 3 、R 4 、R 5 The same or different, independently of each other, from a substituted or unsubstituted alkyl group, a substituted or unsubstituted alkenyl group or a substituted or unsubstituted aryl group; if substituted, the substituent is alkyl;
n is an integer between 1 and 3.
According to an embodiment of the invention, R 1 、R 2 、R 3 、R 4 、R 5 Identical or different, independently of one another, from substituted or unsubstituted C 1-12 Alkyl, substituted or unsubstituted C 2-12 Alkenyl or substituted or unsubstituted C 6-18 An aryl group; in the case of substitution, the substituent is C 1-12 An alkyl group.
According to an embodiment of the invention, R 1 、R 2 、R 3 、R 4 、R 5 Identical or different, independently of one another, from substituted or unsubstituted C 1-6 Alkyl, substituted or unsubstituted C 2-6 Alkenyl or substituted or unsubstituted C 6-14 An aryl group; in the case of substitution, the substituent is C 1-6 An alkyl group.
According to an embodiment of the invention, R 1 、R 2 、R 3 、R 4 、R 5 Identical or different, independently of one another, from substituted or unsubstituted C 1-3 Alkyl, substituted or unsubstituted C 2-3 Alkenyl or substituted or unsubstituted C 6-8 An aryl group; in the case of substitution, the substituent is C 1-3 An alkyl group.
According to an embodiment of the invention, n is 1,2 or 3.
According to an embodiment of the present invention, the alkenylsiloxane-based compound has at least one of compounds represented by formulas T1 to T8;
according to the embodiment of the invention, the mass ratio of the alkenyl siloxane compound to the total mass of the electrolyte is 0.1-1.5 wt%; for example 0.1wt%, 0.2wt%, 0.3wt%, 0.4wt%, 0.5wt%, 0.6wt%, 0.7wt%, 0.8wt%, 0.9wt%, 1.0wt%, 1.1wt%, 1.2wt%, 1.3wt%, 1.4wt% or 1.5wt%.
According to the embodiment of the invention, the mass ratio of the lithium difluorooxalato borate to the total mass of the electrolyte is 0.2-1.2 wt%; for example 0.2wt%, 0.3wt%, 0.4wt%, 0.5wt%, 0.6wt%, 0.7wt%, 0.8wt%, 0.9wt%, 1.0wt%, 1.1wt% or 1.2wt%.
According to the embodiment of the invention, the mass ratio of the lithium bistrifluoromethylsulfonyl imide to the total mass of the electrolyte is 0.5-5 wt%; for example 0.5wt%, 0.6wt%, 0.7wt%, 0.8wt%, 0.9wt%, 1.0wt%, 1.1wt%, 1.2wt%, 1.3wt%, 1.4wt%, 1.5wt%, 1.6wt%, 1.8wt%, 2wt%, 2.2wt%, 2.5wt%, 2.8wt%, 3wt%, 3.2wt%, 3.5wt%, 3.8wt%, 4wt%, 4.2wt%, 4.5wt%, 4.8wt% or 5wt%.
In accordance with an embodiment of the present invention, the second fluorinated solvent comprises fluoroethylene carbonate (FEC), methyl trifluoroethyl carbonate (FEMC), 1, 2-tetrafluoroethyl-2, 3-tetrafluoropropyl ether (TTE) at least one of fluorodiethyl carbonate (FDEC), ethyl 2, 2-trifluoroacetate (FEA), 1, 2-tetrafluoroethyl-2, 2-trifluoroethyl ether (HFE) and 1, 4-difluorobenzene.
According to the embodiment of the invention, the mass ratio of the first fluorinated solvent to the total mass of the electrolyte is 5-30 wt%; for example 5wt%, 6wt%, 8wt%, 10wt%, 12wt%, 13wt%, 15wt%, 16wt%, 18wt%, 20wt%, 22wt%, 25wt%, 28wt% or 30wt%.
According to the embodiment of the invention, the mass ratio of the second fluorinated solvent to the total mass of the electrolyte is 5-20 wt%; for example 5wt%, 6wt%, 8wt%, 10wt%, 12wt%, 13wt%, 15wt%, 16wt%, 18wt% or 20wt%.
According to an embodiment of the invention, the organic solvent further comprises ethyl propionate.
According to the embodiment of the invention, the mass ratio of the ethyl propionate to the total mass of the electrolyte is 5-60 wt%; for example 5wt%, 10wt%, 15wt%, 20wt%, 25wt%, 30wt%, 35wt%, 40wt%, 45wt%, 50wt%, 55wt% or 60wt%.
According to an embodiment of the invention, the additive further comprises a second additive selected from potassium 5-formylthiophene-2-trifluoroborate.
According to the embodiment of the invention, the mass ratio of the second additive to the total mass of the electrolyte is 0.2-1.5 wt%; for example 0.2wt%, 0.3wt%, 0.4wt%, 0.5wt%, 0.6wt%, 0.7wt%, 0.8wt%, 0.9wt%, 1.0wt%, 1.1wt%, 1.2wt%, 1.3wt%, 1.4wt% or 1.5wt%.
According to an embodiment of the present invention, the additive further comprises a third additive selected from at least one of tris (trimethylsilyl) phosphite, tris (trimethylsilyl) borate, lithium difluorosulfimide, 1, 3-propane sultone, 1, 3-propenolactone, vinyl sulfite, vinyl sulfate, vinylene carbonate, and vinyl carbonate.
According to an embodiment of the present invention, the mass ratio of the third additive to the total mass of the electrolyte is 1 to 15wt%, for example, 1wt%, 2wt%, 3wt%, 4wt%, 5wt%, 6wt%, 7wt%, 8wt%, 9wt%, 10wt%, 11wt%, 12wt%, 13wt%, 14wt% or 15wt%.
According to an embodiment of the present invention, the organic solvent further includes at least one of Ethylene Carbonate (EC), propylene Carbonate (PC), dimethyl carbonate, diethyl carbonate, methylethyl carbonate, propyl Propionate (PP), and propyl acetate.
According to an embodiment of the present invention, the electrolyte lithium salt is selected from at least one of lithium difluorosulfonimide and lithium hexafluorophosphate.
According to an embodiment of the present invention, the electrolyte salt is present in an amount of 13wt% to 20wt%, such as 13wt%, 14wt%, 15wt%, 16wt%, 17wt%, 18wt%, 19wt% or 20wt%, based on the total mass of the electrolyte.
The invention also provides a battery, which comprises the electrolyte.
According to an embodiment of the invention, the battery is a lithium ion battery.
According to an embodiment of the present invention, the battery further includes a positive electrode, a negative electrode, and a separator.
According to an embodiment of the present invention, the positive electrode sheet includes a positive electrode current collector and a positive electrode active material layer coated on one or both side surfaces of the positive electrode current collector, the positive electrode active material layer including a positive electrode active material, a conductive agent, and a binder.
According to an embodiment of the present invention, the positive electrode active material is selected from lithium cobaltate or lithium cobaltate subjected to a doping coating treatment of two or more elements of Al, mg, mn, cr, ti, zr, and the chemical formula of the lithium cobaltate subjected to the doping coating treatment of two or more elements of Al, mg, mn, cr, ti, zr is Li x Co 1-y1-y2-y3-y4 A y1 B y2 C y3 D y4 O 2 The method comprises the steps of carrying out a first treatment on the surface of the X is more than or equal to 0.95 and less than or equal to 1.05,0.01, y1 is more than or equal to 0.1, y2 is more than or equal to 0.01 and less than or equal to 0.1, y3 is more than or equal to 0 and less than or equal to 0.1, y4 is more than or equal to 0 and less than or equal to 0.1, and A and B, C, D are selected from two or more elements of Al, mg, mn, cr, ti, zr.
According to an embodiment of the present invention, the negative electrode sheet includes a negative electrode current collector and a negative electrode active material layer coated on one or both side surfaces of the negative electrode current collector, the negative electrode active material layer including a negative electrode active material, a conductive agent, and a binder.
According to an embodiment of the present invention, the negative electrode active material is selected from graphite; and optionally SiOx/C or Si/C, wherein 0< x <2.
According to an embodiment of the present invention, the positive electrode active material layer comprises the following components in percentage by mass: 80 to 99.8 weight percent of positive electrode active material, 0.1 to 10 weight percent of conductive agent and 0.1 to 10 weight percent of binder.
Preferably, the positive electrode active material layer comprises the following components in percentage by mass: 90 to 99.6 weight percent of positive electrode active material, 0.2 to 5 weight percent of conductive agent and 0.2 to 5 weight percent of binder.
According to an embodiment of the present invention, the mass percentage of each component in the anode active material layer is: 80 to 99.8 weight percent of negative electrode active material, 0.1 to 10 weight percent of conductive agent and 0.1 to 10 weight percent of binder.
Preferably, the mass percentage of each component in the anode active material layer is as follows: 90 to 99.6 weight percent of negative electrode active material, 0.2 to 5 weight percent of conductive agent and 0.2 to 5 weight percent of binder.
According to an embodiment of the present invention, the conductive agent is at least one selected from conductive carbon black, acetylene black, ketjen black, conductive graphite, conductive carbon fiber, carbon nanotube, and metal powder.
According to an embodiment of the present invention, the binder is at least one selected from sodium carboxymethyl cellulose, styrene-butadiene latex, polytetrafluoroethylene, and polyethylene oxide.
The invention has the beneficial effects that:
the invention provides an electrolyte and a battery comprising the same, wherein the electrolyte adopts a fluoro solvent and the combination of alkenyl siloxane compounds, lithium difluoro oxalato borate and lithium bis (trifluoromethyl) sulfonyl imide; when the alkenyl siloxane compound is singly used, a protective film can be formed on the surfaces of the anode and the cathode, but the impedance of the protective film is larger and the ionic conductivity is lower; when the lithium difluorooxalate and the lithium bistrifluoromethylsulfonyl imide are combined, the lithium bistrifluoromethylsulfonyl imide contains larger anions and is easier to dissociate, so that the ionic conductivity can be improved, the lithium difluorooxalate and alkenyl siloxane compounds form a composite interface protection film on the surface of the positive electrode and the negative electrode, the composite interface protection film is firm, the interface compatibility of the electrode and the electrolyte can be improved, the three can act together, the composite interface protection film generated on the surface of the positive electrode and the negative electrode is firm and has lower impedance, the side reaction between the electrode and the electrolyte is effectively inhibited, the lithium bistrifluorosulfonate electrolyte has the characteristic of high ionic conductivity, and the high-voltage stability of the electrolyte can be further improved by matching with a fluorinated solvent with better oxidation resistance, so that the safety performance (the thermal shock performance, the overcharge performance and the needling performance can be simultaneously considered), and the high-temperature cycle performance and the low-temperature performance of the battery under high voltage are also improved.
On the basis, the further introduced second additive (5-formylthiophene-2-potassium trifluoroborate) can strengthen the synergistic effect among the additives in the electrolyte, and when the second additive is combined with the first additive and the fluorinated solvent, a high-strength composite interface protective film can be generated on the surface of the positive electrode, and the trifluoroborate is an electron-withdrawing functional group, so that the electrolyte has higher oxidation stability, can improve the high-voltage resistance of the electrolyte and promote Li + The solvation of the electrolyte is caused to change, the solvation sheath layer is changed, the lithium ion migration number is higher, the conductivity of the electrolyte can be improved, the electrochemical stability of the electrolyte is obviously improved while the low-temperature performance of the battery is improved, the electrolyte is more resistant to high voltage and is not flammable, and the safety performance of the battery is further improved.
On the basis, the further introduced third additive can also participate in film forming, and acts on the surfaces of the positive electrode and the negative electrode to form a composite interface protection film, so that the electrochemical stability of the electrolyte is stabilized, and the performance of the battery is improved.
Detailed Description
The present invention will be described in further detail with reference to specific examples. It is to be understood that the following examples are illustrative only and are not to be construed as limiting the scope of the invention. All techniques implemented based on the above description of the invention are intended to be included within the scope of the invention.
The experimental methods used in the following examples are all conventional methods unless otherwise specified; the reagents, materials, etc. used in the examples described below are commercially available unless otherwise specified.
Comparative examples 1 to 5 and examples 1 to 12
The lithium ion batteries of comparative examples 1 to 5 and examples 1 to 12 were each prepared according to the following preparation method, except that the solvent, the additive were selected and the addition amount was different, and the specific differences are shown in table 1.
(1) Preparation of positive plate
LiCoO as positive electrode active material 2 Mixing polyvinylidene fluoride (PVDF) as a binder and acetylene black as a conductive agent according to a weight ratio of 97.5:1.5:1, adding N-methylpyrrolidone (NMP), and stirring under the action of a vacuum stirrer until the mixed system becomes anode slurry with uniform fluidity; uniformly coating the anode slurry on an aluminum foil with the thickness of 10 mu m; and baking the coated aluminum foil in 5 sections of ovens with different temperature gradients, drying the aluminum foil in an oven with the temperature of 120 ℃ for 8 hours, and rolling and slitting the aluminum foil to obtain the required positive plate.
(2) Preparation of negative plate
The preparation method comprises the steps of preparing a slurry from 97.5% by mass of artificial graphite anode material, 0.2% by mass of single-walled carbon nanotube (SWCNT) conductive agent, 0.5% by mass of conductive carbon black (SP) conductive agent, 0.5% by mass of sodium carboxymethylcellulose (CMC) binder and 1.3% by mass of Styrene Butadiene Rubber (SBR) binder by a wet process, coating the slurry on the surface of a copper foil of an anode current collector, and drying (temperature: 85 ℃ C., time: 5 h), rolling and die cutting to obtain the anode sheet.
(3) Electrolyte preparation
In a glove box filled with argon (moisture)<10ppm, oxygen content<1 ppm), ethylene Carbonate (EC), propylene Carbonate (PC) and Propyl Propionate (PP) were uniformly mixed in a mass ratio of 1:1:3, and 14wt.% LiPF based on the total mass of the electrolyte was slowly added to the mixed solution 6 3wt.% of 1, 3-propenolactone, additives (alkenylsiloxanes, lithium difluorooxalato borate, lithium bistrifluoromethylsulfonimide and potassium 5-formylthiophene-2-trifluoroborate), fluorosolvents and ethyl propionate (specific amounts and choices of additives, fluorosolvents and ethyl propionate)As shown in table 1), and stirring uniformly to obtain an electrolyte.
(4) Preparation of separator
A polyethylene separator having a thickness of 5 μm was coated with a composite layer of a mixture of titanium oxide and polyvinylidene fluoride-hexafluoropropylene copolymer having a thickness of 2 μm.
(5) Preparation of lithium ion batteries
Winding the prepared positive plate, diaphragm and negative plate to obtain a bare cell without liquid injection; and placing the bare cell in an outer packaging foil, injecting the prepared electrolyte into the dried bare cell, and performing the procedures of vacuum packaging, standing, formation, shaping, sorting and the like to obtain the required lithium ion battery.
TABLE 1 composition of electrolyte for lithium ion batteries prepared in comparative examples 1 to 5 and examples 1 to 12
Electrochemical performance tests were performed on the lithium ion batteries obtained in the above comparative examples and examples, and are described below:
(1) 45 ℃ cycle experiment: placing the batteries obtained in the examples and the comparative examples in an environment with the temperature of (45+/-2), standing for 2-3 hours, charging the battery to the cutoff current of 4.5V according to the constant current of 1C to be 0.05C when the battery body reaches the temperature of (45+/-2), standing for 5 minutes after the battery is fully charged, discharging to the cutoff voltage of 3.0V according to the constant current of 0.5C, recording the highest discharge capacity of the previous 3 times of circulation as initial capacity Q, and recording the discharge capacity Q of the last time of the battery when the circulation reaches the required times 1 The results are recorded in table 2.
The calculation formula used therein is as follows: capacity retention (%) =q 1 /Q×100％。
(2) Low temperature discharge experiment: the batteries obtained in the above examples and comparative examples were subjected to a temperature of 0.2 at ambient temperature (25.+ -. 3 ℃ C.)C, discharging to 3.0V, and standing for 5min; charging with 0.7C, changing into constant voltage charging when the voltage of the battery cell terminal reaches 4.5V, stopping current being 0.05C, standing for 5min, discharging with 0.2C to 3.0V, recording that the discharge capacity is normal temperature capacity Q 2 . Then the battery cell is charged at 0.7C, when the voltage of the battery cell end reaches 4.5V, constant voltage charging is changed, and the cut-off current is 0.05C; after the fully charged battery is placed for 4 hours under the condition of (-20+/-2) DEG C, the battery is discharged to the cut-off voltage of 3.0V by 0.2C current, and the discharge capacity Q is recorded 3 The low-temperature discharge capacity retention rate was calculated and the results are shown in table 2.
Low-temperature discharge capacity retention rate (%) =q of battery 3 /Q 2 ×100％。
(3) Thermal shock test at 132 ℃): the batteries obtained in the above examples and comparative examples were heated by convection or a circulating hot air box at an initial temperature of (25.+ -. 3), a temperature change rate of (5.+ -. 2) DEG C/min, and the temperature was raised to (132.+ -. 2) DEG C, and after holding for 60 minutes, the test was ended, and the battery state results were recorded as shown in Table 2.
(4) Overfill experiments: the batteries obtained in the above examples and comparative examples were charged at a constant current at 3C rate to a 5V recording battery state, and the recording results are shown in table 2.
(5) Performing needling experiments; the battery obtained in the above examples and comparative examples was penetrated by a high temperature resistant steel needle having a diameter phi of 5-8 mm (conical angle of needle tip is 45-60 ℃, surface of needle is smooth and clean and free from rust, oxide layer and oil stain) at a speed of (25 + -5) mm/s from the direction perpendicular to the battery plate, and the penetration position is preferably near the geometric center of the penetrated surface (steel needle stays in the battery). The test was stopped and the battery state was recorded when the highest temperature of the battery surface was lowered to the peak temperature of 10 c or below for 1 hour, and the results were recorded as shown in table 2.
Table 2 results of experimental tests on batteries obtained in comparative examples 1 to 5 and examples 1 to 12
From the results in table 2, it can be seen that: according to the invention, the safety performance of the lithium ion battery can be obviously improved through the synergistic effect between the fluorogenic solvent, the alkenyl siloxane compound, the lithium difluorooxalato borate and the lithium bistrifluoromethylsulfonyl imide by adding the fluorogenic solvent, the alkenyl siloxane compound, the lithium difluorooxalato borate and the lithium bistrifluoromethylsulfonyl imide into the electrolyte, and the high-temperature cycle performance and the low-temperature performance of the battery under high voltage are improved.
The embodiments of the present invention have been described above. However, the present invention is not limited to the above embodiment. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. An electrolyte, characterized in that the electrolyte comprises an organic solvent, an additive and an electrolyte salt; the additive comprises a first additive selected from the group consisting of alkenylsiloxanes, lithium difluorooxalato borate, and lithium bistrifluoromethylsulfonimide;
the organic solvent comprises a fluorinated solvent; the fluorinated solvent comprises a first fluorinated solvent and a second fluorinated solvent; the first fluorinated solvent is selected from ethyl 2, 2-difluoroacetate; the second fluorinated solvent includes at least one of a fluorinated carbonate, a fluorinated carboxylate, a fluoroether, and a fluorobenzene.
2. The electrolyte of claim 1, wherein the alkenyl siloxane compound is an alkenyl-containing siloxane compound.
Preferably, the alkenyl siloxane compound has a structural formula shown in a formula I:
in the formula I, R 1 、R 2 、R 3 、R 4 、R 5 The same or different, independently of each other, from a substituted or unsubstituted alkyl group, a substituted or unsubstituted alkenyl group or a substituted or unsubstituted aryl group; if substituted, the substituent is alkyl;
n is an integer between 1 and 3.
3. The electrolyte according to claim 1 or 2, wherein the mass ratio of the alkenylsiloxane compound to the total mass of the electrolyte is 0.1wt% to 1.5wt%.
4. The electrolyte according to any one of claims 1 to 3, wherein the mass ratio of the lithium difluorooxalato borate to the total mass of the electrolyte is 0.2 to 1.2wt%;
and/or the mass ratio of the lithium bistrifluoromethylsulfonylimide to the total mass of the electrolyte is 0.5-5 wt%.
5. The electrolyte according to any one of claim 1 to 4, wherein, the second fluorinated solvent comprises fluoroethylene carbonate (FEC), methyl trifluoroethyl carbonate (FEMC), 1, 2-tetrafluoroethyl-2, 3-tetrafluoropropyl ether (TTE) at least one of fluorodiethyl carbonate (FDEC), ethyl 2, 2-trifluoroacetate (FEA), 1, 2-tetrafluoroethyl-2, 2-trifluoroethyl ether (HFE) and 1, 4-difluorobenzene.
6. The electrolyte according to any one of claims 1 to 5, wherein the mass ratio of the first fluorinated solvent to the total mass of the electrolyte is 5 to 30wt%;
and/or the mass ratio of the second fluorinated solvent to the total mass of the electrolyte is 5-20wt%.
7. The electrolyte according to any one of claims 1 to 6, wherein the organic solvent further comprises ethyl propionate;
and/or the mass ratio of the ethyl propionate to the total mass of the electrolyte is 5-60 wt%.
8. The electrolyte of any one of claims 1-7 wherein the additive further comprises a second additive selected from the group consisting of potassium 5-formylthiophene-2-trifluoroborate;
and/or the mass ratio of the second additive to the total mass of the electrolyte is 0.2-1.5 wt%.
9. The electrolyte of any one of claims 1-8 wherein the additive further comprises a third additive selected from at least one of tris (trimethylsilyl) phosphite, tris (trimethylsilyl) borate, lithium bis-fluorosulfonimide, 1, 3-propane sultone, 1, 3-propenoic acid lactone, vinyl sulfite, vinyl sulfate, vinylene carbonate, and vinyl carbonate;
and/or the mass ratio of the third additive to the total mass of the electrolyte is 1-15 wt%.
10. A battery comprising the electrolyte of any one of claims 1-9.
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