CN111477962B - Non-aqueous electrolyte of lithium ion battery and lithium ion battery containing non-aqueous electrolyte - Google Patents
Non-aqueous electrolyte of lithium ion battery and lithium ion battery containing non-aqueous electrolyte Download PDFInfo
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- CN111477962B CN111477962B CN202010482249.6A CN202010482249A CN111477962B CN 111477962 B CN111477962 B CN 111477962B CN 202010482249 A CN202010482249 A CN 202010482249A CN 111477962 B CN111477962 B CN 111477962B
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 56
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 56
- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 23
- 239000003792 electrolyte Substances 0.000 claims abstract description 40
- -1 thiouracil compound Chemical class 0.000 claims abstract description 38
- 229950000329 thiouracil Drugs 0.000 claims abstract description 26
- 239000000654 additive Substances 0.000 claims abstract description 17
- 230000000996 additive effect Effects 0.000 claims abstract description 16
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 12
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 11
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 11
- 125000004430 oxygen atom Chemical group O* 0.000 claims abstract description 6
- 125000004434 sulfur atom Chemical group 0.000 claims abstract description 6
- 239000008151 electrolyte solution Substances 0.000 claims abstract description 5
- 239000004215 Carbon black (E152) Substances 0.000 claims abstract description 4
- 150000001335 aliphatic alkanes Chemical class 0.000 claims abstract description 4
- 125000002915 carbonyl group Chemical class [*:2]C([*:1])=O 0.000 claims abstract description 4
- 150000001875 compounds Chemical class 0.000 claims abstract description 4
- 125000004185 ester group Chemical class 0.000 claims abstract description 4
- 229910052736 halogen Inorganic materials 0.000 claims abstract description 4
- 150000002367 halogens Chemical class 0.000 claims abstract description 4
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims abstract description 4
- 125000002560 nitrile group Chemical class 0.000 claims abstract description 4
- 229910052717 sulfur Chemical group 0.000 claims abstract description 4
- 229910052744 lithium Inorganic materials 0.000 claims description 21
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 12
- 229910019142 PO4 Inorganic materials 0.000 claims description 11
- 239000012752 auxiliary agent Substances 0.000 claims description 11
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 11
- 239000010452 phosphate Substances 0.000 claims description 11
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 10
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 9
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 claims description 9
- 239000007774 positive electrode material Substances 0.000 claims description 9
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 8
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 8
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims description 8
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 8
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 7
- XNENYPKLNXFICU-UHFFFAOYSA-N P(O)(O)O.C[SiH](C)C.C[SiH](C)C.C[SiH](C)C Chemical compound P(O)(O)O.C[SiH](C)C.C[SiH](C)C.C[SiH](C)C XNENYPKLNXFICU-UHFFFAOYSA-N 0.000 claims description 7
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 7
- ZRZFJYHYRSRUQV-UHFFFAOYSA-N phosphoric acid trimethylsilane Chemical compound C[SiH](C)C.C[SiH](C)C.C[SiH](C)C.OP(O)(O)=O ZRZFJYHYRSRUQV-UHFFFAOYSA-N 0.000 claims description 7
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 6
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 5
- HNAGHMKIPMKKBB-UHFFFAOYSA-N 1-benzylpyrrolidine-3-carboxamide Chemical compound C1C(C(=O)N)CCN1CC1=CC=CC=C1 HNAGHMKIPMKKBB-UHFFFAOYSA-N 0.000 claims description 5
- 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 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 5
- OBNCKNCVKJNDBV-UHFFFAOYSA-N butanoic acid ethyl ester Natural products CCCC(=O)OCC OBNCKNCVKJNDBV-UHFFFAOYSA-N 0.000 claims description 5
- 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 5
- 239000007773 negative electrode material Substances 0.000 claims description 5
- 229910052757 nitrogen Inorganic materials 0.000 claims description 5
- DKPFZGUDAPQIHT-UHFFFAOYSA-N Butyl acetate Natural products CCCCOC(C)=O DKPFZGUDAPQIHT-UHFFFAOYSA-N 0.000 claims description 4
- 229910052782 aluminium Inorganic materials 0.000 claims description 4
- FUZZWVXGSFPDMH-UHFFFAOYSA-N hexanoic acid Chemical compound CCCCCC(O)=O FUZZWVXGSFPDMH-UHFFFAOYSA-N 0.000 claims description 4
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 4
- 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 4
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 claims description 4
- 229920002554 vinyl polymer Polymers 0.000 claims description 4
- HJGJHDZQLWWMRT-UHFFFAOYSA-N 2,2,2-trifluoroethyl hydrogen carbonate Chemical compound OC(=O)OCC(F)(F)F HJGJHDZQLWWMRT-UHFFFAOYSA-N 0.000 claims description 3
- 229910052796 boron Inorganic materials 0.000 claims description 3
- 229910052804 chromium Inorganic materials 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- FFYPMLJYZAEMQB-UHFFFAOYSA-N diethyl pyrocarbonate Chemical compound CCOC(=O)OC(=O)OCC FFYPMLJYZAEMQB-UHFFFAOYSA-N 0.000 claims description 3
- 229910052733 gallium Inorganic materials 0.000 claims description 3
- 229910052749 magnesium Inorganic materials 0.000 claims description 3
- 229910052748 manganese Inorganic materials 0.000 claims description 3
- 229910052712 strontium Inorganic materials 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 229910052725 zinc Inorganic materials 0.000 claims description 3
- DSMUTQTWFHVVGQ-UHFFFAOYSA-N 4,5-difluoro-1,3-dioxolan-2-one Chemical compound FC1OC(=O)OC1F DSMUTQTWFHVVGQ-UHFFFAOYSA-N 0.000 claims description 2
- 238000006864 oxidative decomposition reaction Methods 0.000 abstract description 5
- 230000000694 effects Effects 0.000 abstract description 4
- 238000006243 chemical reaction Methods 0.000 abstract description 3
- 125000002813 thiocarbonyl group Chemical group *C(*)=S 0.000 abstract description 3
- 102100028667 C-type lectin domain family 4 member A Human genes 0.000 description 12
- 101000766908 Homo sapiens C-type lectin domain family 4 member A Proteins 0.000 description 12
- 239000000203 mixture Substances 0.000 description 12
- 230000000052 comparative effect Effects 0.000 description 8
- 238000012360 testing method Methods 0.000 description 8
- 230000014759 maintenance of location Effects 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- 238000001035 drying Methods 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 238000005260 corrosion Methods 0.000 description 3
- 230000007797 corrosion Effects 0.000 description 3
- 238000005520 cutting process Methods 0.000 description 3
- 238000011161 development Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229910021382 natural graphite Inorganic materials 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- ZQAZPYAZPAMCGH-UHFFFAOYSA-N 2-sulfooxyethyl hydrogen sulfate Chemical compound OS(=O)(=O)OCCOS(O)(=O)=O ZQAZPYAZPAMCGH-UHFFFAOYSA-N 0.000 description 2
- DDEWVRFHURYTHA-UHFFFAOYSA-N 5-fluoro-1,3-dimethylpyrimidine-2,4-dione Chemical compound CN1C=C(F)C(=O)N(C)C1=O DDEWVRFHURYTHA-UHFFFAOYSA-N 0.000 description 2
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 2
- ISAKRJDGNUQOIC-UHFFFAOYSA-N Uracil Natural products O=C1C=CNC(=O)N1 ISAKRJDGNUQOIC-UHFFFAOYSA-N 0.000 description 2
- AJYQMCHCOGIXMR-IDTAVKCVSA-N [(2r,3s,4r,5r)-5-[6-(4-bromo-2,3-dioxobutyl)sulfanylpurin-9-yl]-3,4-dihydroxyoxolan-2-yl]methyl phosphono hydrogen phosphate Chemical compound O[C@@H]1[C@H](O)[C@@H](COP(O)(=O)OP(O)(O)=O)O[C@H]1N1C2=NC=NC(SCC(=O)C(=O)CBr)=C2N=C1 AJYQMCHCOGIXMR-IDTAVKCVSA-N 0.000 description 2
- 239000010405 anode material Substances 0.000 description 2
- 239000006256 anode slurry Substances 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 239000002041 carbon nanotube Substances 0.000 description 2
- 229910021393 carbon nanotube Inorganic materials 0.000 description 2
- 239000006258 conductive agent Substances 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 238000004146 energy storage Methods 0.000 description 2
- 238000009472 formulation Methods 0.000 description 2
- 230000008014 freezing Effects 0.000 description 2
- 238000007710 freezing Methods 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 229920003048 styrene butadiene rubber Polymers 0.000 description 2
- ZEMGGZBWXRYJHK-UHFFFAOYSA-N thiouracil Chemical compound O=C1C=CNC(=S)N1 ZEMGGZBWXRYJHK-UHFFFAOYSA-N 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- 229940035893 uracil Drugs 0.000 description 2
- 238000003466 welding Methods 0.000 description 2
- RGUQUFJUZGFSNC-UHFFFAOYSA-N 1,2-difluoroethenyl hydrogen carbonate Chemical compound C(=C(OC(=O)O)F)F RGUQUFJUZGFSNC-UHFFFAOYSA-N 0.000 description 1
- NAJMIVLMDLWNRF-UHFFFAOYSA-N 2-methylbutyl hydrogen carbonate Chemical compound CCC(C)COC(O)=O NAJMIVLMDLWNRF-UHFFFAOYSA-N 0.000 description 1
- 229910020784 Co0.2O2 Inorganic materials 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910013716 LiNi Inorganic materials 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 239000002174 Styrene-butadiene Substances 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- HFCVPDYCRZVZDF-UHFFFAOYSA-N [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O Chemical compound [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O HFCVPDYCRZVZDF-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
- 230000001070 adhesive effect Effects 0.000 description 1
- 239000002671 adjuvant Substances 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- 239000007767 bonding agent Substances 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000000839 emulsion Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000003446 memory effect Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 239000002153 silicon-carbon composite material Substances 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 238000009966 trimming 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
- H01M10/42—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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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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)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- Physics & Mathematics (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention provides a lithium ion battery non-aqueous electrolyte and a lithium ion battery containing the same, the non-aqueous electrolyte comprises lithium salt, a non-aqueous organic solvent and an additive, the additive comprises a thiouracil compound, the mass percentage of the thiouracil compound in the electrolyte is 0.01-5%, the structural formula of the thiouracil compound is as follows,
wherein X is oxygen atom or sulfur atom, R1, R2, R3 and R4 are respectively and independently selected from halogen, hydrogen group and C1‑C6Hydrocarbon compound of (2), C1‑C6And (3) halogenated alkane, nitrile group, ester group and carbonyl group. The thiouracil compound can optimize the interface between the positive electrode and the electrolyte, reduce the surface activity of the positive electrode and inhibit the oxidative decomposition of the electrolyte. the-N-structure can be complexed with F-to absorb HF formed by reaction, and can effectively avoid electrolyte Solution (SEI) and CEI films from being corroded and reformed to consume electrolyte solution, thereby improving the cycle performance; the thiocarbonyl structure enables a formed film to be thinner, more flexible and lower in impedance, and contributes to improvement of low-temperature performance.
Description
Technical Field
The invention relates to the field of lithium ion batteries, and relates to a lithium ion battery non-aqueous electrolyte and a lithium ion battery containing the same.
Background
The lithium ion battery has the advantages of high specific energy, no memory effect, long cycle life and the like, and is widely applied to the fields of 3C digital, electric tools, aerospace, energy storage, power automobiles and the like, and the rapid development of electronic information technology and consumer products puts higher requirements on the high voltage and high energy density of the lithium ion battery. In lithium ion batteries, high-voltage ternary positive electrode materials (NCM or NCA) are widely applied to portable electronic devices such as mobile phones and notebook computers, electric vehicles and large energy storage devices due to the advantages of high energy density, environmental friendliness, long cycle life and the like, but the energy density of batteries is higher and higher in the market, so that the commercial ternary positive electrode material lithium ion batteries are difficult to meet the use requirements.
At present, research shows that one of effective ways for improving the energy density of the ternary electrode material is to improve the working voltage of the battery, which is a trend of battery development and is also an inevitable requirement for new energy automobile development. However, after the working voltage of the ternary power battery is increased, the performances of the battery, such as charge and discharge cycles, are reduced. The reasons may be: on one hand, the anode material is not stable enough under high voltage, on the other hand, the matching property of the electrolyte and the material is not good, and the common electrolyte can be oxidized and decomposed under the condition of high voltage, so that the battery has poor high-temperature storage performance, poor high-temperature cycle performance, poor low-temperature discharge performance and poor safety, therefore, the research and development of the lithium ion battery electrolyte suitable for a high-voltage ternary material system is urgent.
Disclosure of Invention
The invention aims to provide a lithium ion battery non-aqueous electrolyte and a lithium ion battery containing the same, wherein the electrolyte can improve the cycle and low-temperature performance of the battery, and is particularly suitable for the lithium ion battery under a high-voltage system.
In order to achieve the above object, a first aspect of the present invention provides a lithium ion battery nonaqueous electrolyte, including a lithium salt, a nonaqueous organic solvent, and an additive, where the additive includes a thiouracil compound, a mass percentage of the thiouracil compound in the electrolyte is 0.01 to 5%, a structural formula of the thiouracil compound is as follows,
wherein X is oxygen atom or sulfur atom, R1, R2, R3 and R4 are respectively and independently selected from halogen, hydrogen group and C1-C6Hydrocarbon compound of (2), C1-C6And (3) halogenated alkane, nitrile group, ester group and carbonyl group.
Compared with the prior art, the additive of the non-aqueous electrolyte of the lithium ion battery comprises 0.01-5% of thiouracil compound, and the use of the thiouracil compound can optimize the interface between the positive electrode and the electrolyte, reduce the surface activity of the positive electrode, and inhibit the oxidative decomposition of the electrolyte. the-N-structure can be complexed with F-to absorb HF formed by reaction, so that electrolyte solution can be effectively prevented from being consumed due to corrosion and reformation of SEI and CEI films, and the cycle performance of the battery is improved; and the thiocarbonyl structure is thinner in formed film, is more flexible and lower in impedance, and contributes to improving the low-temperature performance of the lithium ion battery. Therefore, the uracil compound with a special structure is adopted, so that the battery cycle performance can be improved, and the low-temperature performance can be considered.
Further, the mass percentage of the thiouracil compound in the electrolyte is 0.01-0.5%.
Further, the thiouracil compound is selected from one of the following formulas 1 to 7,
further, the lithium salt is selected from at least one of lithium hexafluorophosphate, lithium difluorophosphate, lithium bis (oxalato) borate, lithium difluoro (oxalato) phosphate, lithium tetrafluoroborate, lithium tetrafluorooxalato phosphate, lithium bis (trifluoromethylsulfonyl) imide and lithium bis (fluorosulfonyl) imide.
Further, the non-aqueous organic solvent is selected from at least one of ethylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, propylene carbonate, butyl acetate, gamma-butyrolactone, propyl propionate, ethyl propionate and ethyl butyrate.
The electrolyte further comprises 0.1-10.5% by mass of an auxiliary agent in the electrolyte, wherein the auxiliary agent is selected from at least one of 2,2, 2-trifluoroethyl carbonate, 2,2, 2-diethyl trifluorocarbonate, 2,2, 2-ethylpropyl trifluorocarbonate, fluoroethylene carbonate, vinylene carbonate, diethyl pyrocarbonate, 1, 3-propane sultone, vinyl sulfate, 1, 2-difluoroethylene carbonate, tris (trimethylsilane) phosphate, tris (trimethylsilane) phosphite, 4 '-bi-1, 3-dioxolane-2, 2' -dione, 3-divinyl bissulfate and 4, 4-vinyl bisdisulfate.
Further, the auxiliary agent is at least one of vinylene carbonate, 1, 3-propane sulfonic acid lactone, vinyl sulfate, tris (trimethylsilane) phosphate, tris (trimethylsilane) phosphite, 4 '-bi-1, 3-dioxolane-2, 2' -dione, 3-ethylene bissulfate and 4, 4-ethylene bissulfate.
The invention also provides a lithium ion battery, which comprises a positive electrode material, a negative electrode material and an electrolyte, wherein the electrolyte is the lithium ion battery non-aqueous electrolyte, and the maximum charging voltage is 4.4V.
The lithium ion battery adopts the uracil compound with a special structure as an additive of the electrolyte, and the electrolyte can optimize the interface of the positive electrode and the electrolyte under a high-voltage system with the charging voltage of 4.4V, reduce the surface activity of the positive electrode and inhibit the oxidative decomposition of the electrolyte. A low-impedance and stable CEI film can be formed on the surface of the anode, and the transition metal in the anode material is prevented from being oxidized, so that the transition metal is prevented from dissolving out, and the reversibility of charge and discharge in circulation is improved; can absorb HF, can effectively avoid the consumption of electrolyte caused by the corrosion and reformation of SEI and CEI films; and the film forming impedance is lower and the film forming resistance is more flexible, thereby being beneficial to simultaneously improving the cycle performance and the low-temperature performance of the lithium ion battery.
Further, the cathode material is Li(1+a)NixCoyMzN1-x-y-zO2+bWherein M is Mn or Al, N is any one of Mg, Cu, Zn, Sn, B, Ga, Cr, Sr, Ba, V and Ti, a is more than-0.10 and less than or equal to 0.50, x is more than 0 and less than 1, y is more than 0 and less than 1, 0 and less than 0<z＜1，0.7＜x+y+z≤1，-0.05≤b≤0.10。
Detailed Description
The invention provides a lithium ion battery non-aqueous electrolyte, which comprises lithium salt, a non-aqueous organic solvent and an additive, wherein the additive comprises a thiouracil compound, the mass percentage of the thiouracil compound in the electrolyte is 0.01-5%, the structural formula of the thiouracil compound is as follows,
wherein X is oxygen atom or sulfur atom, R1, R2, R3 and R4 are respectively and independently selected from halogen, hydrogen group and C1-C6Hydrocarbon compound of (2), C1-C6And (3) halogenated alkane, nitrile group, ester group and carbonyl group.
The thiouracil compound may be present in an amount of, but not limited to, 0.01%, 0.1%, 0.5%, 1%, 1.5%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%. Preferably, the mass percentage of the thiouracil compound in the electrolyte is 0.01-0.5%.
The thiouracil compound may be selected from, but not limited to, one of the following formulas 1 to 7,
the content of the lithium salt accounts for 10-20% of the total mass of the lithium salt, the non-aqueous organic solvent and the additive, and specifically, but not limited to, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%. The lithium salt may be specifically selected from at least one of lithium hexafluorophosphate, lithium difluorophosphate, lithium bis (oxalato) borate, lithium difluoro (oxalato) phosphate, lithium tetrafluoroborate, lithium tetrafluorooxalato phosphate, lithium bis (trifluoromethylsulfonyl) imide and lithium bis (fluorosulfonyl) imide. Preferably, the lithium bis (oxalato) borate and the lithium difluoro (oxalato) borate are mixed, the lithium difluoro (oxalato) borate and the lithium difluoro (oxalato) phosphate are mixed, the lithium difluoro (oxalato) phosphate and the lithium tetrafluorooxalato phosphate are mixed, the lithium tetrafluorooxalato phosphate and the lithium bis (trifluoromethylsulfonyl) imide are mixed, the lithium bis (trifluoromethylsulfonyl) imide and the lithium bis (fluorosulfonyl) imide are mixed, the lithium tetrafluoroborate and the lithium difluorophosphates are mixed, and the lithium bis (oxalato) borate, the lithium difluoro (oxalato) borate and the lithium difluoro (oxalato) phosphate are mixed.
The nonaqueous organic solvent accounts for 60-80% of the total mass of the lithium salt, the nonaqueous organic solvent and the additive, and may be, but is not limited to, 60%, 65%, 66%, 67%, 68%, 69%, 70%, 71%, 72%, 73%, 74%, 75%, 80%. The non-aqueous organic solvent is at least one selected from the group consisting of Ethylene Carbonate (EC), dimethyl carbonate (DMC), diethyl carbonate (DEC), Ethyl Methyl Carbonate (EMC), Propylene Carbonate (PC), butyl acetate (n-BA), gamma-butyrolactone (GBL), propyl propionate (n-PP), Ethyl Propionate (EP) and Ethyl Butyrate (EB). Preferably, the mixture of ethylene carbonate and dimethyl carbonate, the mixture of dimethyl carbonate and diethyl carbonate, the mixture of diethyl carbonate and ethyl methyl carbonate, the mixture of ethyl methyl carbonate and propylene carbonate, the mixture of propylene carbonate and gamma-butyrolactone, the mixture of gamma-butyrolactone and propyl propionate, the mixture of propyl propionate and ethyl propionate, the mixture of dimethyl carbonate, diethyl carbonate and ethyl methyl carbonate, and the mixture of ethyl butyrate and butyl acetate.
The electrolyte also comprises 0.1-10.5% of an auxiliary agent by mass, wherein the auxiliary agent is selected from at least one of 2,2, 2-trifluoroethyl carbonate, 2,2, 2-ethylpropyl carbonate, fluoroethylene carbonate (FEC), Vinylene Carbonate (VC), diethyl pyrocarbonate, 1, 3-Propane Sultone (PS), vinyl sulfate (DTD), 1, 2-difluorovinyl carbonate, tris (trimethylsilane) phosphate (TMSP), tris (trimethylsilane) phosphite (TTMSPi), 4 '-bi-1, 3-dioxolane-2, 2' -dione (BDC), 3-divinyl Bissulfate (BDTD) and 4, 4-vinyl bisdisulfate. Preferably, the auxiliary agent is selected from vinylene carbonate, 1, 3-propane sulfonic acid lactone, vinyl sulfate, tris (trimethylsilane) phosphate, tris (trimethylsilane) phosphite, 4 '-bi-1, 3-dioxolane-2, 2' -dione, 3-divinyl bi sulfate or 4, 4-divinyl bi-sulfate, and the content is 0.1-2%, 0.2-2%, 0.1-1.5% and 0.1-1.5% respectively. The electrolyte is characterized in that vinyl sulfate (DTD) is added into the electrolyte as an auxiliary agent, the surface SEI film component can be modified, the relative content of sulfur atoms and oxygen atoms is improved, the sulfur atoms and the oxygen atoms contain lone-pair electrons and can attract lithium ions, the shuttle of the lithium ions in the SEI film is accelerated, the interface impedance of the battery is reduced, and therefore the low-temperature charge and discharge performance of the high-voltage lithium ion battery is effectively improved. The 1, 3-Propane Sultone (PS) as an auxiliary agent has good film-forming property and low-temperature conductivity, can inhibit the decomposition of FEC, and improves the capacity loss of the lithium ion battery during the first charge and discharge, thereby being beneficial to improving the reversible capacity of the lithium ion battery and further improving the long-term cycle performance of the lithium ion battery. The tris (trimethylsilane) phosphate (TMSP) and the tris (trimethylsilane) phosphite (TTMSPi) can absorb moisture and free acid, and the cycle performance of the battery is improved.
The invention provides a lithium ion battery, which comprises a positive electrode material, a negative electrode material and an electrolyte, wherein the electrolyte is the lithium ion battery non-aqueous electrolyte, and the maximum charging voltage is 4.4V. Wherein the positive electrode material is Li(1+a)NixCoyMzN1-x-y-zO2+bWherein M is Mn or Al, N is any one of Mg, Cu, Zn, Sn, B, Ga, Cr, Sr, Ba, V and Ti, a is more than-0.10 and less than or equal to 0.50, x is more than 0 and less than 1, 0 and less than 0<z is less than 1, x + y + z is more than 0.7 and less than or equal to 1, and b is more than or equal to 0.05 and less than or equal to 0.10. The negative electrode material is any one of artificial graphite, natural graphite, lithium titanate, a silicon-carbon composite material and silicon monoxide.
To better illustrate the objects, technical solutions and advantages of the present invention, the present invention will be further described with reference to specific examples. It should be noted that the following implementation of the method is a further explanation of the present invention, and should not be taken as a limitation of the present invention.
Example 1
In a nitrogen-filled glove box (O)2＜2ppm，H2O < 3ppm), dimethyl carbonate, diethyl carbonate and ethyl methyl carbonate are uniformly mixed according to the mass ratio of 3:5:2 to prepare 79.7g of a nonaqueous organic solvent, and 0.3g of formula 1 is added as an additive to prepare a mixed solution. Sealing, packaging, freezing at a freezing room (-4 deg.C) for 2 hr, taking out, and placing in a nitrogen-filled glove box (O)2＜2ppm，H2O is less than 3ppm), 20g of lithium hexafluorophosphate is slowly added into the mixed solution, and the electrolyte is prepared after uniform mixing.
The formulations of the electrolytes of examples 2 to 20 and comparative examples 1 to 4 are shown in Table 1, and the procedure for preparing the electrolyte is the same as that of example 1.
TABLE 1 electrolyte formulation of the examples
Wherein, the comparative example 4 is 5-fluoro-1, 3-dimethyluracil, and the structural formula is shown as the following formula 8.
The lithium ion battery is prepared by using the NCM523 with the highest charging voltage of 4.4V as a positive electrode material and natural graphite as a negative electrode material and by using the electrolytes of examples 1 to 20 and comparative examples 1 to 4 according to the following lithium battery preparation method, and normal-temperature cycle performance, high-temperature cycle performance and low-temperature discharge test are respectively carried out.
The preparation method of the lithium ion battery comprises the following steps:
1. preparation of positive plate
LiNi prepared from nickel cobalt lithium manganate ternary material0.5Mn0.3Co0.2O2Uniformly mixing the conductive agent SuperP, the adhesive PVDF and the Carbon Nano Tubes (CNT) according to the mass ratio of 97.5:1.5:1:1 to prepare lithium ion battery anode slurry with certain viscosity, and coating the lithium ion battery anode slurry on an aluminum foil for a current collector, wherein the coating weight is 324g/m2Drying at 85 ℃ and then carrying out cold pressing; and then trimming, cutting into pieces, slitting, drying for 4h at 85 ℃ under a vacuum condition after slitting, and welding tabs to prepare the lithium ion battery positive plate meeting the requirements.
2. Preparing a negative plate: preparing natural graphite, a conductive agent SuperP, a thickening agent CMC and a bonding agent SBR (styrene butadiene rubber emulsion) into slurry according to the mass ratio of 95:1.4:1.4:2.2, coating the slurry on a current collector copper foil, and drying at 85 ℃, wherein the coating weight is 168g/m2(ii) a And (3) cutting edges, cutting pieces, slitting, drying for 4h at 110 ℃ under a vacuum condition after slitting, and welding tabs to prepare the lithium ion battery negative plate meeting the requirements.
3. Preparing a lithium ion battery: and (3) preparing the positive plate, the negative plate and the diaphragm prepared by the process into a lithium ion battery with the thickness of 4.7mm, the width of 55mm and the length of 60mm by a lamination process, baking the lithium ion battery for 10 hours at 75 ℃, and injecting the non-aqueous electrolyte. After standing for 24h, the mixture was charged to 4.45V with a constant current of 0.lC (180mA), and then charged at a constant voltage of 4.45V until the current dropped to 0.05C (90 mA); then discharging to 3.0V with 0.2C (180mA), repeating the charging and discharging for 2 times, finally charging the battery to 3.8V with 0.2C (180mA), and finishing the manufacture of the battery.
The test conditions of the normal temperature cycle performance, the high temperature cycle performance and the low temperature discharge test are as follows, and the test results are shown in table 2.
And (3) testing the normal-temperature cycle performance:
the lithium ion battery is placed in an environment with the temperature of 25 ℃, is charged to 4.4V by a current of 1C at a constant current, is charged at a constant voltage until the current is reduced to 0.05C, is discharged to 3.0V by a current of 1C at a constant current, is circulated, and is measured for DCIR every 50 circles. The discharge capacity of the first and last turn was recorded, as well as the DCIR every 50 turns. The capacity retention and DCIR increase for the high temperature cycle were calculated as follows.
Capacity retention rate ═ last cycle discharge capacity/first cycle discharge capacity × 100%
DCIR lift ═ DCIR of last 50 cycles/DCIR of first cycle × 100%
And (3) testing high-temperature cycle performance:
the cell was placed in an oven at a constant temperature of 45C, constant current charged to 4.4V at 1C and then constant voltage charged to 0.05C, and then constant current discharged to 3.0V at 1C, cycled through this cycle, and then DCIR was measured every 50 cycles. The discharge capacity of the first and last turn was recorded, as well as the DCIR every 50 turns. The capacity retention and DCIR increase for the high temperature cycle were calculated as follows.
Capacity retention rate ═ last cycle discharge capacity/first cycle discharge capacity × 100%
DCIR lift ═ DCIR of last 50 cycles/DCIR of first cycle × 100%
And (3) low-temperature discharge test:
the battery was charged at a constant current of 0.5C to 4.4V at normal temperature and then charged at a constant voltage until the current dropped to 0.05C, and then placed in a thermostat at a constant temperature of-20℃ and discharged at a constant current of 0.5C to 3.0V.
Battery capacity retention (%) retention capacity/initial capacity × 100%
TABLE 2 results of cycle and Low temperature Performance testing
From the results in Table 2, it is understood that examples 1 to 20 are superior to comparative examples 1 to 4 in both high-temperature and normal-temperature cycle performance and low-temperature discharge performance. The additive of the non-aqueous electrolyte of the lithium ion battery comprises 0.01-5% of thiouracil compound, and the use of the thiouracil compound can optimize the interface between the positive electrode and the electrolyte, reduce the surface activity of the positive electrode and inhibit the oxidative decomposition of the electrolyte. the-N-structure can be complexed with F-to absorb HF formed by reaction, so that electrolyte solution can be effectively prevented from being consumed due to corrosion and reformation of SEI and CEI films, and the cycle performance of the battery is improved; and the thiocarbonyl structure is thinner in formed film, is more flexible and lower in impedance, and contributes to improving the low-temperature performance of the lithium ion battery. In contrast, comparative example 1, only a nonaqueous organic solvent and a lithium salt are used as an electrolyte, and thus the problems of instability of the positive electrode material at a high voltage and oxidative decomposition of the electrolyte at a high voltage cannot be solved, resulting in poor cycle performance and low temperature performance. Comparative example 2 using only VC as an aid improved the cycle performance to some extent, but the low temperature performance was poor. Comparative example 3 using only FEC as an aid can improve low temperature performance to some extent, but the cycle performance in high voltage systems is far from ideal. Although the 5-fluoro-1, 3-dimethyluracil of comparative example 4 also has an-N-structure, and can capture hydrofluoric acid and prevent decomposition of an electrolyte at high temperature, the film forming is thicker, the impedance is higher, and the low-temperature performance is obviously insufficient compared with the thiouracil additive of the present invention, and although the high-temperature performance of the lithium ion battery can be improved to a certain extent, the low-temperature performance cannot be considered, and the cycle performance is also slightly insufficient.
It can be seen from comparison of example 1 and examples 13-20 that the cycle performance and low temperature performance are better when some additives (such as FEC, DTD, TMSP, TTMSPi, BDTD) are added on the basis of the thiouracil additive. Although the low temperature performance is reduced after the addition of the VC and PS adjuvants, the cycle performance at normal and high temperatures is better than that of example 1.
Finally, it should be noted that the above embodiments are only used for illustrating the technical solutions of the present invention and not for limiting the protection scope of the present invention, and although the present invention is described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that modifications or equivalent substitutions can be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention.
Claims (9)
1. The lithium ion battery non-aqueous electrolyte comprises lithium salt, a non-aqueous organic solvent and an additive, and is characterized in that the additive comprises a thiouracil compound, the mass percentage of the thiouracil compound in the electrolyte is 0.01-5%, the structural formula of the thiouracil compound is as follows,
wherein X is oxygen atom or sulfur atom, R1, R2, R3 and R4 are respectively and independently selected from halogen, hydrogen group and C1-C6Hydrocarbon compound of (2), C1-C6And (3) halogenated alkane, nitrile group, ester group and carbonyl group.
2. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the mass percentage of the thiouracil compound in the electrolyte solution is 0.01 to 0.5%.
3. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the thiouracil compound is one selected from the group consisting of the following formulae 1 to 7,
4. the nonaqueous electrolyte for lithium ion batteries according to claim 1, wherein the lithium salt is at least one selected from the group consisting of lithium hexafluorophosphate, lithium difluorophosphate, lithium bis (oxalato) borate, lithium difluoro (oxalato) phosphate, lithium tetrafluoroborate, lithium tetrafluorooxalato phosphate, lithium bis (trifluoromethylsulfonyl) imide and lithium bis (fluorosulfonyl) imide.
5. The nonaqueous electrolyte for lithium ion batteries according to claim 1, wherein the nonaqueous organic solvent is at least one selected from the group consisting of ethylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, propylene carbonate, butyl acetate, γ -butyrolactone, propyl propionate, ethyl propionate, and ethyl butyrate.
6. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1, further comprising an auxiliary agent in an amount of 0.1 to 10.5% by mass, the auxiliary agent is at least one selected from 2,2, 2-trifluoroethyl carbonate, 2,2, 2-diethyl trifluorocarbonate, 2,2, 2-ethylpropyl trifluorocarbonate, fluoroethylene carbonate, vinylene carbonate, diethyl pyrocarbonate, 1, 3-propane sultone, vinyl sulfate, 1, 2-difluoroethylene carbonate, tris (trimethylsilane) phosphate, tris (trimethylsilane) phosphite, 4 '-bi-1, 3-dioxolane-2, 2' -dione, 3-divinyl bissulfate and 4, 4-vinyl bissulfate.
7. The nonaqueous electrolyte solution for lithium ion batteries according to claim 6, wherein the auxiliary agent is at least one of vinylene carbonate, 1, 3-propane sultone, vinyl sulfate, tris (trimethylsilane) phosphate, tris (trimethylsilane) phosphite, 4 '-bi-1, 3-dioxolane-2, 2' -dione, 3-divinyl bissulfate, and 4, 4-vinyl bisulphate.
8. A lithium ion battery comprising a positive electrode material, a negative electrode material and an electrolyte, wherein the electrolyte is the lithium ion battery nonaqueous electrolyte according to any one of claims 1 to 7, and the maximum charging voltage is 4.4V.
9. The lithium ion battery of claim 8, wherein the positive electrode material is Li(1+a)NixCoyMzN1-x-y- zO2+bWherein M is Mn or Al, N is any one of Mg, Cu, Zn, Sn, B, Ga, Cr, Sr, Ba, V and Ti, a is more than-0.10 and less than or equal to 0.50, x is more than 0 and less than 1, y is more than 0 and less than 1, 0 and less than 0<z＜1，0.7＜x+y+z≤1，-0.05≤b≤0.10。
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