CN114024036A - Low-concentration lithium ion battery electrolyte and lithium ion battery prepared from same - Google Patents
Low-concentration lithium ion battery electrolyte and lithium ion battery prepared from same Download PDFInfo
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- CN114024036A CN114024036A CN202111307387.1A CN202111307387A CN114024036A CN 114024036 A CN114024036 A CN 114024036A CN 202111307387 A CN202111307387 A CN 202111307387A CN 114024036 A CN114024036 A CN 114024036A
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- lithium
- carbonate
- ion battery
- lithium ion
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 73
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 72
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 72
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 33
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 33
- 239000006184 cosolvent Substances 0.000 claims abstract description 16
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 13
- 229910052744 lithium Inorganic materials 0.000 claims description 26
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 20
- -1 lithium hexafluorophosphate Chemical compound 0.000 claims description 16
- 239000002904 solvent Substances 0.000 claims description 13
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 12
- YMWUJEATGCHHMB-UHFFFAOYSA-N Dichloromethane Chemical compound ClCCl YMWUJEATGCHHMB-UHFFFAOYSA-N 0.000 claims description 11
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 9
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 9
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 9
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 8
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-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
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 7
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 7
- NMJJFJNHVMGPGM-UHFFFAOYSA-N butyl formate Chemical compound CCCCOC=O NMJJFJNHVMGPGM-UHFFFAOYSA-N 0.000 claims description 6
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 claims description 5
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 4
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 claims description 4
- 125000003709 fluoroalkyl group Chemical group 0.000 claims description 4
- KGPPDNUWZNWPSI-UHFFFAOYSA-N flurotyl Chemical compound FC(F)(F)COCC(F)(F)F KGPPDNUWZNWPSI-UHFFFAOYSA-N 0.000 claims description 4
- 150000008282 halocarbons Chemical class 0.000 claims description 4
- ZQBFAOFFOQMSGJ-UHFFFAOYSA-N hexafluorobenzene Chemical compound FC1=C(F)C(F)=C(F)C(F)=C1F ZQBFAOFFOQMSGJ-UHFFFAOYSA-N 0.000 claims description 4
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 4
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 4
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 4
- VNXYDFNVQBICRO-UHFFFAOYSA-N 1,1,1,3,3,3-hexafluoro-2-methoxypropane Chemical compound COC(C(F)(F)F)C(F)(F)F VNXYDFNVQBICRO-UHFFFAOYSA-N 0.000 claims description 3
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 claims description 3
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 3
- SJHAYVFVKRXMKG-UHFFFAOYSA-N 4-methyl-1,3,2-dioxathiolane 2-oxide Chemical compound CC1COS(=O)O1 SJHAYVFVKRXMKG-UHFFFAOYSA-N 0.000 claims description 3
- DKPFZGUDAPQIHT-UHFFFAOYSA-N Butyl acetate Natural products CCCCOC(C)=O DKPFZGUDAPQIHT-UHFFFAOYSA-N 0.000 claims description 3
- FERIUCNNQQJTOY-UHFFFAOYSA-M Butyrate Chemical compound CCCC([O-])=O FERIUCNNQQJTOY-UHFFFAOYSA-M 0.000 claims description 3
- WBJINCZRORDGAQ-UHFFFAOYSA-N formic acid ethyl ester Natural products CCOC=O WBJINCZRORDGAQ-UHFFFAOYSA-N 0.000 claims description 3
- FUZZWVXGSFPDMH-UHFFFAOYSA-N hexanoic acid Chemical compound CCCCCC(O)=O FUZZWVXGSFPDMH-UHFFFAOYSA-N 0.000 claims description 3
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 3
- 229940090181 propyl acetate Drugs 0.000 claims description 3
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 claims description 3
- WACNXHCZHTVBJM-UHFFFAOYSA-N 1,2,3,4,5-pentafluorobenzene Chemical compound FC1=CC(F)=C(F)C(F)=C1F WACNXHCZHTVBJM-UHFFFAOYSA-N 0.000 claims description 2
- SOZFIIXUNAKEJP-UHFFFAOYSA-N 1,2,3,4-tetrafluorobenzene Chemical compound FC1=CC=C(F)C(F)=C1F SOZFIIXUNAKEJP-UHFFFAOYSA-N 0.000 claims description 2
- AJKNNUJQFALRIK-UHFFFAOYSA-N 1,2,3-trifluorobenzene Chemical compound FC1=CC=CC(F)=C1F AJKNNUJQFALRIK-UHFFFAOYSA-N 0.000 claims description 2
- GOYDNIKZWGIXJT-UHFFFAOYSA-N 1,2-difluorobenzene Chemical compound FC1=CC=CC=C1F GOYDNIKZWGIXJT-UHFFFAOYSA-N 0.000 claims description 2
- ZPFAVCIQZKRBGF-UHFFFAOYSA-N 1,3,2-dioxathiolane 2,2-dioxide Chemical compound O=S1(=O)OCCO1 ZPFAVCIQZKRBGF-UHFFFAOYSA-N 0.000 claims description 2
- DJXNLVJQMJNEMN-UHFFFAOYSA-N 2-[difluoro(methoxy)methyl]-1,1,1,2,3,3,3-heptafluoropropane Chemical compound COC(F)(F)C(F)(C(F)(F)F)C(F)(F)F DJXNLVJQMJNEMN-UHFFFAOYSA-N 0.000 claims description 2
- FNUBKINEQIEODM-UHFFFAOYSA-N 3,3,4,4,5,5,5-heptafluoropentanal Chemical compound FC(F)(F)C(F)(F)C(F)(F)CC=O FNUBKINEQIEODM-UHFFFAOYSA-N 0.000 claims description 2
- 125000000217 alkyl group Chemical group 0.000 claims description 2
- DISYGAAFCMVRKW-UHFFFAOYSA-N butyl ethyl carbonate Chemical compound CCCCOC(=O)OCC DISYGAAFCMVRKW-UHFFFAOYSA-N 0.000 claims description 2
- FWBMVXOCTXTBAD-UHFFFAOYSA-N butyl methyl carbonate Chemical compound CCCCOC(=O)OC FWBMVXOCTXTBAD-UHFFFAOYSA-N 0.000 claims description 2
- VASVAWIFVXAQMI-UHFFFAOYSA-N butyl propyl carbonate Chemical compound CCCCOC(=O)OCCC VASVAWIFVXAQMI-UHFFFAOYSA-N 0.000 claims description 2
- 125000004432 carbon atom Chemical group C* 0.000 claims description 2
- QLVWOKQMDLQXNN-UHFFFAOYSA-N dibutyl carbonate Chemical compound CCCCOC(=O)OCCCC QLVWOKQMDLQXNN-UHFFFAOYSA-N 0.000 claims description 2
- HSNQKJVQUFYBBY-UHFFFAOYSA-N dipentyl carbonate Chemical compound CCCCCOC(=O)OCCCCC HSNQKJVQUFYBBY-UHFFFAOYSA-N 0.000 claims description 2
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 claims description 2
- BQZQELQEOWCZLR-UHFFFAOYSA-N ethyl pentyl carbonate Chemical compound CCCCCOC(=O)OCC BQZQELQEOWCZLR-UHFFFAOYSA-N 0.000 claims description 2
- CYEDOLFRAIXARV-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound CCCOC(=O)OCC CYEDOLFRAIXARV-UHFFFAOYSA-N 0.000 claims description 2
- PAQGTCFSKWUKHW-UHFFFAOYSA-N methyl pentyl carbonate Chemical compound CCCCCOC(=O)OC PAQGTCFSKWUKHW-UHFFFAOYSA-N 0.000 claims description 2
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-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
- SCSDLMBSTOZBPZ-UHFFFAOYSA-N pentyl propyl carbonate Chemical compound CCCCCOC(=O)OCCC SCSDLMBSTOZBPZ-UHFFFAOYSA-N 0.000 claims description 2
- 238000007614 solvation Methods 0.000 abstract description 5
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 abstract description 3
- 239000003063 flame retardant Substances 0.000 abstract description 3
- 239000007774 positive electrode material Substances 0.000 abstract description 3
- 239000010405 anode material Substances 0.000 abstract description 2
- 239000010406 cathode material Substances 0.000 abstract description 2
- 238000004880 explosion Methods 0.000 abstract description 2
- 239000003963 antioxidant agent Substances 0.000 abstract 1
- 230000003078 antioxidant effect Effects 0.000 abstract 1
- 238000009736 wetting Methods 0.000 abstract 1
- 230000000052 comparative effect Effects 0.000 description 21
- 238000012360 testing method Methods 0.000 description 10
- JDZCKJOXGCMJGS-UHFFFAOYSA-N [Li].[S] Chemical compound [Li].[S] JDZCKJOXGCMJGS-UHFFFAOYSA-N 0.000 description 4
- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical compound COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 description 4
- 238000011056 performance test Methods 0.000 description 4
- 210000004027 cell Anatomy 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 229910013075 LiBF Inorganic materials 0.000 description 2
- 229910013872 LiPF Inorganic materials 0.000 description 2
- 101150058243 Lipf gene Proteins 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
- 239000006256 anode slurry Substances 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000003085 diluting agent Substances 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- GBPVMEKUJUKTBA-UHFFFAOYSA-N methyl 2,2,2-trifluoroethyl carbonate Chemical compound COC(=O)OCC(F)(F)F GBPVMEKUJUKTBA-UHFFFAOYSA-N 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- HCBRSIIGBBDDCD-UHFFFAOYSA-N 1,1,2,2-tetrafluoro-3-(1,1,2,2-tetrafluoroethoxy)propane Chemical compound FC(F)C(F)(F)COC(F)(F)C(F)F HCBRSIIGBBDDCD-UHFFFAOYSA-N 0.000 description 1
- 229910015013 LiAsF Inorganic materials 0.000 description 1
- 229910010710 LiFePO Inorganic materials 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- FLIHROUXKOLBTC-UHFFFAOYSA-N butyl pentyl carbonate Chemical compound CCCCCOC(=O)OCCCC FLIHROUXKOLBTC-UHFFFAOYSA-N 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 239000006258 conductive agent Substances 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 238000004807 desolvation Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000012983 electrochemical energy storage Methods 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 239000013538 functional additive Substances 0.000 description 1
- 239000012442 inert solvent Substances 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 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 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- ZDCRNXMZSKCKRF-UHFFFAOYSA-N tert-butyl 4-(4-bromoanilino)piperidine-1-carboxylate Chemical compound C1CN(C(=O)OC(C)(C)C)CCC1NC1=CC=C(Br)C=C1 ZDCRNXMZSKCKRF-UHFFFAOYSA-N 0.000 description 1
- 125000001889 triflyl group Chemical group FC(F)(F)S(*)(=O)=O 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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Classifications
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- 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
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
-
- 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
- H01M2300/0088—Composites
- H01M2300/0091—Composites in the form of mixtures
-
- 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
Abstract
The invention discloses a low-concentration lithium ion battery electrolyte and a lithium ion battery prepared from the same. The low-concentration lithium ion battery electrolyte consists of lithium salt, a non-aqueous organic solvent and an inert cosolvent; wherein: the concentration of the lithium salt is 0.1-0.8 mol/L, and the volume ratio of the non-aqueous organic solvent to the inert cosolvent is (20-80): 20-80. The low-concentration lithium ion battery electrolyte has excellent antioxidant stability, and can form a stable interface with a positive electrode material, so that the cycle performance of the lithium ion battery is improved; the electrolyte has a unique lithium ion solvation structure and lower viscosity, so that the electrolyte has good wetting performance with the diaphragm and the anode and cathode materials, and the rate capability of the lithium ion battery can be effectively improved. The electrolyte has good flame retardant property, can improve the safety performance of the lithium ion battery, and reduces the risk of ignition and explosion; and the dosage of lithium salt in the electrolyte is reduced, so that the cost of the electrolyte and the lithium ion battery is greatly reduced.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a low-concentration lithium ion battery electrolyte and a lithium ion battery prepared from the same.
Background
Lithium ion batteries are currently the most widely used clean electrochemical energy storage devices. In recent years, lithium ion batteries have been widely used in portable electronic devices such as mobile phones and notebook computers, and are advancing to the fields of electric vehicles and large-scale energy storage. The electrolyte of the lithium ion battery is an indispensable part of the lithium ion battery and is an important carrier for connecting the anode and the cathode to realize ion transmission. Since the commercialization of lithium ion batteries, conventional lithium ion battery electrolytes have been composed of lithium hexafluorophosphate, ethylene carbonate, linear carbonates (dimethyl carbonate, ethyl methyl carbonate, etc.) and functional additives, wherein the concentration of lithium salt is always fixed at about 1 mol/L. The concentration of 1mol/L is selected mainly because the ion conductivity of most nonaqueous electrolyte systems always reaches a maximum at a concentration of about 1 mol/L.
Compared with the traditional electrolyte, the high-concentration electrolyte has remarkable advantages in performance due to the unique lithium ion solvation structure, and comprises the advantages of effectively inhibiting the formation of lithium dendrites, having a wider electrochemical stability window, having lower volatility, better flame retardant performance and the like. However, the commercial application of the electrolyte is severely limited by the disadvantages of high cost and high viscosity of the electrolyte with high concentration. In order to reduce the viscosity. Zhang Relay Olympic et al (J Electrochem Soc 168:010522.) applied an inert solvent as a diluent to the high concentration electrolyte to form a localized high concentration electrolyte. Because the diluent can not dissolve lithium salt, the obtained local high-concentration electrolyte keeps the solvation structure of lithium ions in the high-concentration electrolyte, thereby inheriting the advantages of wide electrochemical stability window, good flame retardance and the like of the high-concentration electrolyte. However, the concentration of lithium salt in the locally high-concentration electrolyte proposed at present is still about 1mol/L, and although the mass proportion of lithium salt is only 10-12%, the proportion of the cost of the locally high-concentration electrolyte to the total cost of the electrolyte is as high as about 50%.
In patent application publication No. CN109935908A, a low-concentration lithium ion battery electrolyte mixed with lithium salt is reported, and the compatibility of the electrolyte and the electrolyte is improved by selecting lithium salt (lithium bis (oxalato) borate, lithium difluoro (oxalato) borate, etc.) capable of forming a film on the surface of a negative electrode, so as to improve the cycle stability of the lithium ion battery. In the application of patent publication No. CN110911756A, there is reported a lithium-sulfur battery electrolyte of a diluted mixed lithium salt, in which lithium salts (lithium bis (fluorosulfonyl imide), lithium bis (trifluoromethyl sulfonyl imide) and the like) capable of forming films on the surfaces of a positive electrode and a negative electrode are combined to stabilize the lithium negative electrode and the sulfur positive electrode, respectively, thereby improving the cycle stability of the lithium-sulfur battery. However, in order to design an electrolyte from the viewpoint of improving the film formation of an electrode, lithium salts (lithium bis (oxalato) borate, lithium difluoro (oxalato) borate, lithium bis (trifluoromethylsulfonyl) imide, etc.) capable of forming a film on the surface of the electrode must be selected, and the cost of these lithium salts is often much more expensive than that of lithium hexafluorophosphate used in the current commercial electrolyte, and thus, the lithium salts do not have the advantage of large-scale application. In addition, the charge cut-off voltage of the lithium-sulfur battery related in the patent application with publication number of CN110911756A is only 3.0V, which is far lower than the charge cut-off voltage (4.1-4.3V) of the current commercial lithium-ion battery; and thus its application range is relatively narrower. Therefore, low concentration electrolytes developed for current commercial lithium ion batteries must have a higher voltage window than lithium sulfur battery electrolytes. How to reduce the concentration and cost of lithium salt in the lithium ion battery electrolyte and meet the working voltage interval of the lithium ion battery at the same time is a technical problem which needs to be solved urgently.
Disclosure of Invention
The invention aims to provide a low-concentration lithium ion battery electrolyte with lithium salt concentration lower than 0.8mol/L and excellent electrochemical performance and a lithium ion battery prepared from the low-concentration lithium ion battery electrolyte.
The low-concentration lithium ion battery electrolyte consists of lithium salt, a non-aqueous organic solvent and an inert cosolvent; wherein: the concentration of the lithium salt is 0.1-0.8 mol/L, and the volume ratio of the non-aqueous organic solvent to the inert cosolvent is (20-80): 20-80.
Preferably, the concentration of the lithium salt is 0.2-0.6 mol/L; the volume ratio of the non-aqueous organic solvent to the inert cosolvent is (20-50) to (50-80).
The lithium salt is lithium hexafluorophosphate (LiPF)6) Lithium hexafluoroarsenate (LiAsF)6) Lithium tetrafluoroborate (LiBF)4) Lithium perchlorate (LiClO)4) One or more of lithium bistrifluoromethanesulfonylimide (LiTFSI), lithium trifluoromethanesulfonylimide (LiFSI), lithium bis (oxalato) borate (LiBOB) and lithium difluoro (oxalato) borate (lidob).
Preferably, the lithium salt is lithium hexafluorophosphate (LiPF)6) Lithium tetrafluoroborate (LiBF)4) Lithium perchlorate (LiClO)4) One or two of lithium bistrifluoromethanesulfonylimide (LiTFSI), lithium trifluoromethanesulfonylimide (LiFSI), lithium bis (oxalato) borate (LiBOB) and lithium difluoro (oxalato) borate (lidob).
The non-aqueous organic solvent is Ethylene Carbonate (EC), Propylene Carbonate (PC), Butylene Carbonate (BC), fluoroethylene carbonate (FEC), Vinylene Carbonate (VC), dimethyl carbonate (DMC), diethyl carbonate (DEC), Ethyl Methyl Carbonate (EMC), ethyl methyl fluoro carbonate (FEMC), dipropyl carbonate, and methyl propyl carbonate, at least one or more of ethyl propyl carbonate, dibutyl carbonate, methyl butyl carbonate, ethyl butyl carbonate, propyl butyl carbonate, dipentyl carbonate, methyl pentyl carbonate, ethyl pentyl carbonate, propyl pentyl carbonate, butyl pentyl carbonate, Methyl Formate (MF), Ethyl Formate (EF), Propyl Formate (PF), Butyl Formate (BF), Methyl Acetate (MA), Ethyl Acetate (EA), Propyl Acetate (PA), Butyl Acetate (BA), ethylene glycol dimethyl ether (DME), Propylene Sulfite (PS), ethylene sulfate (DTD).
Preferably, the non-aqueous organic solvent is at least one or more of ethylene carbonate, dimethyl carbonate, fluoroethylene carbonate, ethyl methyl carbonate, fluoroethylene carbonate, propylene carbonate and diethyl carbonate.
The inert cosolvent is one or more of hydrofluoroether solvents and halogenated hydrocarbon solvents; wherein:the structural general formula of the hydrofluoroether solvent is R1-O-R2，R1And R2Is an alkyl or fluoroalkyl group having 1 to 10 carbon atoms, and R1And R2Wherein at least one fluoroalkyl group is present; the halogenated hydrocarbon solvent is one or more of fluorobenzene, difluorobenzene, trifluorobenzene, tetrafluorobenzene, pentafluorobenzene, hexafluorobenzene and dichloromethane.
Preferably: the hydrofluoroether solvent is one or more of methyl nonafluorobutyl ether, methyl nonafluoroisobutyl ether, decafluoro-3-methoxy-2-trifluoromethylpentane, hexafluoropropyl methyl ether, 1,2, 2-tetrafluoroethyl-2, 2, 2-trifluoroethyl ether, 1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether, bis (2,2, 2-trifluoroethyl) ether, tetrafluoropropyl methyl ether, 1H, 5H-octafluoropentyl-1, 1,2, 2-tetrafluoroethyl ether and 1,1,2,3,3, 3-pentafluoropropyl-2, 2, 2-trifluoroethyl ether.
A lithium ion battery consists of a positive electrode, a negative electrode, a diaphragm and the low-concentration lithium ion battery electrolyte.
The principle of the invention is as follows: in order to reduce the concentration and cost of lithium salt in the lithium ion battery electrolyte and meet the working voltage interval of the lithium ion battery, the invention firstly proposes to apply an inert cosolvent to the low-concentration lithium ion battery electrolyte from the solvation structure design of lithium ions, improves the voltage window of the low-concentration electrolyte by enhancing the interaction between the lithium ions in the electrolyte and nonaqueous organic solvent molecules, and promotes the desolvation process of the lithium ions by reducing the number of the solvent molecules coordinated with the lithium ions so as to improve the multiplying power performance of the lithium ion battery. The invention reduces the concentration of lithium salt in the lithium ion battery electrolyte, and can directly select the lithium salt which can be commercially applied at present without specially selecting the lithium salt which can form a film on the surface of the anode or the cathode, thereby further reducing the cost of the lithium ion battery electrolyte on the basis of the commercial electrolyte at present.
The invention has the beneficial effects that: 1) the low-concentration lithium ion battery electrolyte has excellent oxidation resistance stability, and can form a stable interface with a positive electrode material, so that the cycle performance of the lithium ion battery is improved. 2) The low-concentration lithium ion battery electrolyte has a unique lithium ion solvation structure, and the rate capability of the lithium ion battery can be effectively improved. 3) The low-concentration lithium ion battery electrolyte has lower viscosity and good infiltration performance with a diaphragm and anode and cathode materials. 4) The low-concentration lithium ion battery electrolyte has good flame retardant property, can improve the safety performance of the lithium ion battery, and reduces the risk of ignition and explosion. 5) The low-concentration lithium ion battery electrolyte can reduce the using amount of lithium salt in the lithium ion battery electrolyte, thereby greatly reducing the cost of the lithium ion battery electrolyte and further reducing the overall cost of the lithium ion battery.
Drawings
Fig. 1 is a graph of the voltage windows of example 1, example 5, comparative example 1, and comparative example 2.
Fig. 2 is a graph of rate performance at normal temperature (25 ℃) of Li | | | | LFP batteries of example 1, example 5, comparative example 1, and comparative example 2.
Fig. 3 is a graph of cycle performance at 1C rate at normal temperature (25 ℃) of the Li | | | LFP batteries of example 1, example 5, comparative example 1, and comparative example 2.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more clearly visible, the present invention is described in more detail with reference to specific examples below. The examples are given solely for the purpose of better illustrating the invention and are not intended to limit the scope of the invention. The lithium salt concentration, the solvent ratio, the formula and the like of the examples can be changed correspondingly according to specific requirements, and the results are not substantially influenced.
Example 1
(1) Preparation of electrolyte
The preparation of the electrolyte is carried out in a glove box which is filled with argon and has the water oxygen content of less than 0.01ppm, firstly ethylene carbonate, dimethyl carbonate and bis (2,2, 2-trifluoroethyl) ether are mixed according to the volume ratio of 1:1:3, and then a certain amount of lithium hexafluorophosphate is added into the mixed solution to obtain the low-concentration lithium ion battery electrolyte with the concentration of 0.3 mol/L.
(2) Testing of electrolyte voltage window
Firstly, a stainless steel sheet | diaphragm | lithium sheet CR2032 button cell filled with the electrolyte is assembled in a glove box, and then a linear volt-ampere scanning test voltage window is carried out on the electrolyte by using an electrochemical workstation (Donghua, DH 7000). The voltage range of the linear scanning is 3V-6V, and the scanning speed is 0.5mV/s
(3) Lithium ion battery assembly and testing
First 0.50g of PVDF was dissolved in 1.45g of NMP to obtain a uniform transparent slurry, and then 0.4g of LiFePO, which is a positive electrode active material, was added4And 0.05g of conductive agent SuperP are added into the transparent slurry and stirred for 6 hours to obtain uniform black anode slurry, then the anode slurry is uniformly coated on an aluminum foil, and the aluminum foil is placed in a vacuum oven for drying at 120 ℃. And cutting the dried positive plate to obtain a positive plate wafer with the diameter of 14mm, and assembling the positive plate wafer, a metal lithium plate (15mm x 0.5mm), a diaphragm (Celgard2320) and the prepared electrolyte into the CR2032 button cell. And (3) adopting a LandBT2001 battery testing system to test the cycle performance and the rate performance of the lithium ion battery, wherein the cycle performance is tested by activating for 2 circles at the rate of 0.2C and then performing 300 circles at the rate of 1C, and the rate performance is tested by circulating for 5 circles at the rates of 0.1C, 0.2C, 0.5C, 1C, 2C, 5C and 0.1C in sequence. The charge-discharge cut-off voltage of the cycle performance and the rate performance test is 2.5V-4.1V.
The compositions of the electrolytes of examples 2 to 12 and comparative examples 1 to 6 are shown in Table 1, and the rest are the same as those of example 1. Wherein: EC means ethylene carbonate, DMC means dimethyl carbonate, EMC means ethyl methyl carbonate, FEC means fluoroethylene carbonate, FEMC means ethyl methyl carbonate, PC means propylene carbonate, DEC means diethyl carbonate, MA means methyl acetate, BTFE means bis (2,2, 2-trifluoroethyl) ether, OTE means 1H, 5H-octafluoropentyl-1, 1,2, 2-tetrafluoroethyl ether, HFE means 1,1,2, 2-tetrafluoroethyl-2, 2, 2-trifluoroethyl ether, TTE means 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether, HFME means hexafluoroisopropyl methyl ether, DCM means dichloromethane.
Table 1: compositions of examples 1 to 12 and comparative examples 1 to 6
The electrolytes of example 1, example 5, comparative example 1 and comparative example 2 were subjected to a voltage window test, and the test results are shown in fig. 1; as can be seen from fig. 1: examples 1 and 5 have a higher voltage window compared to comparative example 1, with example 1 having a higher voltage window even than comparative example 2, indicating that the addition of an inert co-solvent can significantly improve the voltage window of low electrolyte concentrations.
The Li | | | LFP batteries of example 1, example 5, comparative example 1 and comparative example 2 were subjected to a rate performance test at normal temperature (25 ℃), and the test results are shown in fig. 2; as can be seen from fig. 2: example 1 and example 5 exhibited superior rate performance compared to comparative example 1, which demonstrates that the addition of an inert co-solvent can significantly improve the rate performance of Li | | | LFP cells.
The Li | | | LFP batteries of examples 1-12 and comparative examples 1-6 were subjected to 100-cycle 1C cycle performance tests at normal temperature (25 ℃), and the test results are shown in Table 2; from the data in table 2, it can be seen that: the addition of the inert cosolvent can obviously improve the circulation stability of the Li < I > LFP battery in low-concentration electrolyte.
The Li | | | LFP batteries of example 1, example 5, comparative example 1, and comparative example 2 were subjected to a 300-cycle 1C cycle performance test at normal temperature (25 ℃), with the test results shown in fig. 3; as can be seen from fig. 3: the capacity fade of the Li | | | LFP battery was extremely severe in comparative example 1, and even exhibited superior cycle stability in examples 1 and 5 compared to comparative example 2, indicating that the addition of the inert cosolvent can significantly improve the long cycle stability of the Li | | | LFP battery.
Table 2: cycling Performance of examples 1-12 and comparative examples 1-6
Although the invention has been described in general terms and in detail with reference to specific embodiments, it is readily apparent that the invention can be modified or adapted with little effort. It is therefore within the scope of the claimed invention to apply an inert cosolvent (a solvent that is less or incapable of dissolving a lithium salt) to a low concentration lithium ion battery electrolyte without departing from the core of the invention.
Claims (9)
1. The electrolyte of the low-concentration lithium ion battery is characterized by comprising lithium salt, a non-aqueous organic solvent and an inert cosolvent; wherein: the concentration of the lithium salt is 0.1-0.8 mol/L, and the volume ratio of the non-aqueous organic solvent to the inert cosolvent is (20-80): 20-80.
2. The electrolyte for a low-concentration lithium ion battery according to claim 1, wherein the concentration of the lithium salt is 0.2-0.6 mol/L; the volume ratio of the non-aqueous organic solvent to the inert cosolvent is (20-50) to (50-80).
3. The low concentration lithium ion battery electrolyte of claim 1, wherein the lithium salt is one or more of lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium tetrafluoroborate, lithium perchlorate, lithium bistrifluoromethanesulfonylimide, lithium trifluoromethylsulfonyl, lithium bisoxalato borate, and lithium difluorooxalato borate.
4. The low concentration lithium ion battery electrolyte of claim 3, wherein the lithium salt is one or two of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium perchlorate, lithium bistrifluoromethanesulfonylimide, lithium trifluoromethylsulfonyl, lithium bisoxalato borate and lithium difluorooxalato borate.
5. The low-concentration lithium ion battery electrolyte according to claim 1, wherein the non-aqueous organic solvent is at least one or more of ethylene carbonate, propylene carbonate, butylene carbonate, fluoroethylene carbonate, vinylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl fluoro carbonate, dipropyl carbonate, methyl propyl carbonate, ethyl propyl carbonate, dibutyl carbonate, methyl butyl carbonate, ethyl butyl carbonate, propyl butyl carbonate, diamyl carbonate, methyl amyl carbonate, ethyl amyl carbonate, propyl amyl carbonate, butyl formate, ethyl formate, propyl formate, methyl acetate, ethyl acetate, propyl acetate, butyl acetate, ethylene glycol dimethyl ether, propylene sulfite, and ethylene sulfate.
6. The low concentration lithium ion battery electrolyte of claim 5, wherein the non-aqueous organic solvent is one or more of ethylene carbonate, dimethyl carbonate, fluoroethylene carbonate, ethyl methyl carbonate, fluoroethylene carbonate, propylene carbonate, and diethyl carbonate.
7. The electrolyte for the low-concentration lithium ion battery according to claim 1, wherein the inert cosolvent is one or more of a hydrofluoroether solvent and a halogenated hydrocarbon solvent; wherein: the structural general formula of the hydrofluoroether solvent is R1-O-R2，R1And R2Is an alkyl or fluoroalkyl group having 1 to 10 carbon atoms, and R1And R2Wherein at least one fluoroalkyl group is present; the halogenated hydrocarbon solvent is one or more of fluorobenzene, difluorobenzene, trifluorobenzene, tetrafluorobenzene, pentafluorobenzene, hexafluorobenzene and dichloromethane.
8. The low concentration lithium ion battery electrolyte of claim 7, wherein the hydrofluoroether solvent is one or more of methyl nonafluorobutyl ether, methyl nonafluoroisobutyl ether, decafluoro-3-methoxy-2-trifluoromethylpentane, hexafluoropropyl methyl ether, 1,2, 2-tetrafluoroethyl-2, 2, 2-trifluoroethyl ether, 1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether, bis (2,2, 2-trifluoroethyl) ether, tetrafluoropropyl methyl ether, 1H, 5H-octafluoropentyl-1, 1,2, 2-tetrafluoroethyl ether, and 1,1,2,3,3, 3-pentafluoropropyl-2, 2, 2-trifluoroethyl ether.
9. A lithium ion battery, characterized in that it is composed of a positive electrode, a negative electrode, a separator and the low-concentration lithium ion battery electrolyte according to any one of claims 1 to 9.
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