CN105703007A - Non-aqueous electrolyte for high-voltage rapid-charging type lithium ion battery - Google Patents
Non-aqueous electrolyte for high-voltage rapid-charging type lithium ion battery Download PDFInfo
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- CN105703007A CN105703007A CN201610192798.3A CN201610192798A CN105703007A CN 105703007 A CN105703007 A CN 105703007A CN 201610192798 A CN201610192798 A CN 201610192798A CN 105703007 A CN105703007 A CN 105703007A
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- carbonate
- additive
- lithium
- electrolyte
- imide
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- 238000007600 charging Methods 0.000 title claims abstract description 24
- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 19
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 15
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 15
- 239000000654 additive Substances 0.000 claims abstract description 35
- 230000000996 additive effect Effects 0.000 claims abstract description 33
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 32
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 32
- 239000003792 electrolyte Substances 0.000 claims abstract description 21
- 239000002904 solvent Substances 0.000 claims abstract description 20
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 17
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 14
- 150000002825 nitriles Chemical class 0.000 claims abstract description 14
- 239000002000 Electrolyte additive Substances 0.000 claims abstract description 10
- 150000005678 chain carbonates Chemical class 0.000 claims abstract description 7
- 150000005676 cyclic carbonates Chemical group 0.000 claims abstract description 7
- 150000003949 imides Chemical class 0.000 claims abstract description 6
- -1 imide lithium salt Chemical class 0.000 claims description 18
- 239000008151 electrolyte solution Substances 0.000 claims description 13
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 12
- 125000000472 sulfonyl group Chemical group *S(*)(=O)=O 0.000 claims description 10
- 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 7
- MHYFEEDKONKGEB-UHFFFAOYSA-N oxathiane 2,2-dioxide Chemical compound O=S1(=O)CCCCO1 MHYFEEDKONKGEB-UHFFFAOYSA-N 0.000 claims description 7
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 6
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 claims description 6
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 5
- VTHRQKSLPFJQHN-UHFFFAOYSA-N 3-[2-(2-cyanoethoxy)ethoxy]propanenitrile Chemical compound N#CCCOCCOCCC#N VTHRQKSLPFJQHN-UHFFFAOYSA-N 0.000 claims description 5
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 claims description 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 5
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 5
- ZTOMUSMDRMJOTH-UHFFFAOYSA-N glutaronitrile Chemical compound N#CCCCC#N ZTOMUSMDRMJOTH-UHFFFAOYSA-N 0.000 claims description 5
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 claims description 5
- GWAOOGWHPITOEY-UHFFFAOYSA-N 1,5,2,4-dioxadithiane 2,2,4,4-tetraoxide Chemical compound O=S1(=O)CS(=O)(=O)OCO1 GWAOOGWHPITOEY-UHFFFAOYSA-N 0.000 claims description 4
- MXUZSNPHTRQMGP-UHFFFAOYSA-N 4-hydroxybutyl hydrogen sulfate Chemical compound OCCCCOS(O)(=O)=O MXUZSNPHTRQMGP-UHFFFAOYSA-N 0.000 claims description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 4
- 229910013188 LiBOB Inorganic materials 0.000 claims description 4
- 229910013880 LiPF4 Inorganic materials 0.000 claims description 4
- 229910001290 LiPF6 Inorganic materials 0.000 claims description 4
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 claims description 4
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 4
- 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 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 4
- WDXYVJKNSMILOQ-UHFFFAOYSA-N 1,3,2-dioxathiolane 2-oxide Chemical compound O=S1OCCO1 WDXYVJKNSMILOQ-UHFFFAOYSA-N 0.000 claims description 3
- IFDLFCDWOFLKEB-UHFFFAOYSA-N 2-methylbutylbenzene Chemical compound CCC(C)CC1=CC=CC=C1 IFDLFCDWOFLKEB-UHFFFAOYSA-N 0.000 claims description 3
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 claims description 3
- 229910013470 LiC1 Inorganic materials 0.000 claims description 3
- 239000007983 Tris buffer Substances 0.000 claims description 3
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 3
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims description 3
- CYEDOLFRAIXARV-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound CCCOC(=O)OCC CYEDOLFRAIXARV-UHFFFAOYSA-N 0.000 claims description 3
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 claims description 3
- WHULDTBQXVKIHX-UHFFFAOYSA-N propan-2-yl cyanate Chemical compound CC(C)OC#N WHULDTBQXVKIHX-UHFFFAOYSA-N 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
- NEILRVQRJBVMSK-UHFFFAOYSA-N B(O)(O)O.C[SiH](C)C.C[SiH](C)C.C[SiH](C)C Chemical compound B(O)(O)O.C[SiH](C)C.C[SiH](C)C.C[SiH](C)C NEILRVQRJBVMSK-UHFFFAOYSA-N 0.000 claims description 2
- 230000015572 biosynthetic process Effects 0.000 abstract description 5
- 230000003647 oxidation Effects 0.000 abstract description 5
- 238000007254 oxidation reaction Methods 0.000 abstract description 5
- 239000004615 ingredient Substances 0.000 abstract 1
- 230000000052 comparative effect Effects 0.000 description 8
- 238000011056 performance test Methods 0.000 description 8
- 238000012360 testing method Methods 0.000 description 8
- 238000000034 method Methods 0.000 description 5
- 239000007774 positive electrode material Substances 0.000 description 5
- LNLFLMCWDHZINJ-UHFFFAOYSA-N hexane-1,3,6-tricarbonitrile Chemical compound N#CCCCC(C#N)CCC#N LNLFLMCWDHZINJ-UHFFFAOYSA-N 0.000 description 4
- 238000002156 mixing Methods 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 238000000354 decomposition reaction Methods 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 150000002148 esters Chemical class 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- ABDBNWQRPYOPDF-UHFFFAOYSA-N carbonofluoridic acid Chemical compound OC(F)=O ABDBNWQRPYOPDF-UHFFFAOYSA-N 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 206010016766 flatulence Diseases 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical group [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 description 2
- 230000014759 maintenance of location Effects 0.000 description 2
- 239000011268 mixed slurry Substances 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 238000010998 test method Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910012790 LiCoNiMnO2 Inorganic materials 0.000 description 1
- 229910012820 LiCoO Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
- 229910013872 LiPF Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 0.000 description 1
- 229910002097 Lithium manganese(III,IV) oxide Inorganic materials 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 239000004793 Polystyrene Substances 0.000 description 1
- 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 1
- 239000011149 active material Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 150000001408 amides Chemical class 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000005056 compaction Methods 0.000 description 1
- 239000006258 conductive agent Substances 0.000 description 1
- 238000010280 constant potential charging Methods 0.000 description 1
- 238000010277 constant-current charging Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- PGRMNXHYAZYNPG-UHFFFAOYSA-N fluoro hydrogen carbonate Chemical compound OC(=O)OF PGRMNXHYAZYNPG-UHFFFAOYSA-N 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- AHIWWUJXDLMOKI-UHFFFAOYSA-N methoxysulfonylmethanesulfonic acid Chemical compound COS(=O)(=O)CS(O)(=O)=O AHIWWUJXDLMOKI-UHFFFAOYSA-N 0.000 description 1
- PSZYNBSKGUBXEH-UHFFFAOYSA-N naphthalene-1-sulfonic acid Chemical compound C1=CC=C2C(S(=O)(=O)O)=CC=CC2=C1 PSZYNBSKGUBXEH-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 238000006864 oxidative decomposition reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 150000003464 sulfur compounds Chemical class 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- 239000002562 thickening agent Substances 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
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Secondary Cells (AREA)
Abstract
The invention discloses a non-aqueous electrolyte for a high-voltage rapid-charging type lithium ion battery. The non-aqueous electrolyte comprises a solvent, a commonly-used lithium salt, a positive electrode film-forming additive, lithium bis(polyfluoroalkyloxysulfonyl) imide, a fluoro-ester additive, an organic nitrile additive and a lithium battery electrolyte additive, wherein the ingredients are as follows in parts by weight: 100 parts of solvent, 0.2-10 parts of positive electrode film-forming additive, 0.2-10 parts of lithium bis(polyfluoroalkyloxysulfonyl) imide, 0.2-10 parts of fluoro-ester additive and 0.2-10 parts of organic nitrile additive; the solvent is cyclic carbonate and/or chain carbonate; and the molar concentration of the commonly-used lithium salt in the solvent is 0.8-1.5mol/L. According to the non-aqueous electrolyte provided by the invention, the oxidation resistance and wettability of the electrolyte, the oxidation resistance of the positive electrode SEI film in initial formation and the stability of the negative electrode SEI film can be improved; and the normal temperature rapid-charging circulation, the high-temperature 45-DEG C rapid-charging circulation and the high-temperature storage of the high-voltage electrolyte can be greatly improved.
Description
[ technical field ]
The invention relates to an electrolyte of a lithium ion battery, in particular to a non-aqueous electrolyte of a high-voltage quick-charging type lithium ion battery.
[ background art ]
Currently used lithium ion battery positive electrode materials, such as LiCoOO、LiMn2O4,LiCoNiMnO2,LiFePO4The working voltage is lower than 4V, and the gram capacity is 90-150 mg/g. The main methods for increasing the energy density of the battery include 2, one is to increase the charge cut-off voltage of the conventional positive electrode material, for example, the charge voltage of lithium cobaltate is increased to 4.35V and 4.4V, the capacity of the battery can be increased by about 15%, but the method for increasing the charge cut-off voltage is limited, and further increase may lead to poor structural stability when lithium cobaltate is over-delithiated.
However, as the operating voltage and the charge cut-off voltage increase, the oxidation activity of the positive electrode material increases, and the reaction between the positive electrode active material and the electrolyte is accelerated, so that the battery has serious ballooning at high voltage, the cycle performance is reduced, and the performance of the positive electrode material is severely restricted.
[ summary of the invention ]
The invention aims to provide a non-aqueous electrolyte of a high-voltage quick-charging lithium ion battery with excellent charge-discharge cycle performance, so as to improve the normal-temperature quick-charging cycle performance, the high-temperature quick-charging cycle performance at 45 ℃ and the high-temperature storage performance of the lithium ion battery.
In order to solve the technical problems, the invention adopts the technical scheme that the non-aqueous electrolyte of the high-voltage quick-charging lithium ion battery comprises a solvent, a common lithium salt, a positive electrode film-forming additive, a bis (polyfluoroalkoxy sulfonyl) imide lithium salt, a fluorinated ester additive, an organic nitrile additive and a lithium battery electrolyte additive; wherein,
the solvent is cyclic carbonate and/or chain carbonate, and the molar concentration of the common lithium salt in the solvent is 0.8-1.5 mol/L.
In the above nonaqueous electrolytic solution, the cyclic carbonate is at least one of ethylene carbonate, propylene carbonate, fluoroethylene carbonate and γ -butyrolactone.
In the above nonaqueous electrolytic solution, the chain carbonate is at least one of dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, propyl methyl carbonate and propyl ethyl carbonate.
In the above nonaqueous electrolytic solution, the fluorocarbonate additive is fluoroethylene carbonate and/or difluoroethylene carbonate.
The nonaqueous electrolytic solution described above, wherein the lithium bis (polyfluoroalkoxy sulfonyl) imide salt is lithium bis (pentafluoroethyl sulfonyl) imide (Li (C)2F5SO2)2N), lithium trifluoromethylpentafluoroethylsulfonate (Li (CF)3SO2)(C2F5SO2) N), lithium bistrifluoromethylsulfonate (Li (CF)3SO2)2N) and lithium bis (fluorosulfonyl) imide (LiFSI).
The nonaqueous electrolytic solution described above, wherein the organic nitrile is at least one selected from succinonitrile (110-61-2), adiponitrile (111-69-3), glutaronitrile (544-13-8), 3' -oxydipropyronitrile (CAS:1656-48-0), ethylene glycol bis (propionitrile) ether (CAS:3386-87-6), 1,2, 3-tris (2-cyanato) propane (2465-93-2), 1,3, 5-pentanetrimethylnitrile (4379-04-8), 1,2, 3-propanetricitrile (62872-44-0), and 1,3, 6-hexanetrinitrile (1772-25-4).
In the nonaqueous electrolytic solution, the positive electrode film-forming additive is at least one of Vinyl Ethylene Carbonate (VEC), Methylene Methanedisulfonate (MMDS), tris (trimethylsilane) borate (TMSB), tris (trimethylsilane) phosphate (TMSP), and tris (trimethylsilane) phosphate (TMSPi).
The above-mentioned nonaqueous electrolyte solution, wherein the common lithium salt is LiPF6、LiBF4、LiC1O4、LiAsF6LiBOB, LiDFOB and LiPF4C2O4At least one of (1).
The non-aqueous electrolyte comprises a common lithium battery electrolyte additive, wherein the content of the common lithium battery electrolyte additive is 0-10 parts by weight; the common lithium battery electrolyte additive is at least one of Vinylene Carbonate (VC), vinyl sulfate (DTD), Ethylene Sulfite (ES), 1, 3-propane sultone, 1, 3-propene sultone, 1, 4-butane sultone, 1, 4-butanediol sulfate and propenyl-1, 3-sultone.
The invention can improve the oxidation resistance of the electrolyte, the wettability of the electrolyte, the oxidation resistance of a positive electrode SEI film during the primary formation and the stability of a negative electrode SEI film by jointly using the positive electrode film-forming additive, the bis (polyfluoroalkoxy sulfonyl) imide lithium salt fluoro carbonate additive and the organic nitrile additive, and obviously improves the normal-temperature fast-charging circulation, the high-temperature 45-degree fast-charging circulation and the high-temperature storage performance of the high-voltage electrolyte.
[ detailed description of the invention ]
The non-aqueous electrolyte of the high-voltage quick-charging lithium ion battery consists of a solvent, a lithium salt, an additive for improving high-temperature cycle, a bis (polyfluoroalkoxy sulfonyl) imide lithium salt, a fluorinated ester additive, an organic nitrile additive and an additive of the lithium ion battery electrolyte. Wherein, 100 weight portions of solvent; 0.2-10 parts by weight of lithium bis (polyfluoroalkoxy sulfonyl) imide; 0.2-10 parts of high-temperature cycle improving additive; 0.2-10 parts of fluoro carbonate additive; 0.2-10 parts by weight of organic nitrile additive; 0-5 parts of common lithium battery electrolyte additive; the solvent is cyclic carbonate and/or chain carbonate, and the molar concentration of the common lithium salt in the solvent is 0.8-1.5 mol/L.
The lithium bis (polyfluoroalkoxy sulfonyl) imide is used for forming a stable SEI film on the surface of a negative electrode in the formation and circulation processes so as to ensure that the battery has excellent circulation performance, and the formed SEI film contains a sulfur compound and has good thermal stability, so that the battery shows good high-temperature storage performance and high-temperature circulation performance.
The positive electrode film forming additive (high-temperature cycle improving additive) is used for forming a stable SEI film on the surface of a positive electrode in the formation and cycle processes, and has good high-temperature and cycle performances.
The fluoro-carbonate additive is beneficial to improving the reduction potential of solvent molecules on the surface of a carbon cathode, optimizing a solid electrolyte interface film, improving the compatibility of an electrolyte and an active material by means of the electron-withdrawing effect of the F element, further stabilizing the electrochemical performance of an electrode, having better oxidation resistance and being capable of obviously improving the cycle performance of a high-voltage battery.
Although the organic nitrile compound can suppress decomposition of the electrolyte, suppress swelling, and trap dissolved metal ions, the positive electrode resistance increases after the positive electrode is formed into a film, and the cycle performance is lowered. Therefore, the nitrile is added in an amount of 0.2 to 10 parts by weight, and although FEC can improve cycle performance, HF is generated at high temperature and has a catalytic effect on decomposition of an electrolyte solvent, so that the addition of FEC deteriorates high-temperature storage performance of a battery. Therefore, the amount of FEC is selected to be 0.2 to 10 parts by weight.
The organic nitrile substance can absorb a small amount of water and HF to form an amide substance, and HF and POF are reduced3Etc. to cause high-temperature flatulence caused by the decomposition of the electrolyte solvent; nitrile substances can form a stable film on the surface of the anode in the first charge-discharge process, and the anode is effectively inhibited from oxidizing electrolyte, so that high-temperature flatulence is inhibited, and high-temperature storage and cycle performance is improved. The combined use of the four additives can obviously improve the stability of the positive and negative SEI films of the electrolyte under the high-voltage condition, effectively inhibit the oxidative decomposition of the solvent and further improve the cycle performance of the electrolyte under the high-voltage condition.
The common lithium salt is LiPF6、LiBF4、LiC1O4、LiAsF6、、LiBOB，LiDFOB、LiPF4C2O4One or more than two of the components are mixed randomly, and the molar concentration in the solvent is 0.8-1.5 mol/L.
The cyclic carbonate is preferably at least one of Ethylene Carbonate (EC), Propylene Carbonate (PC), fluoroethylene carbonate (FEC) and gamma-butyrolactone (GBL);
the chain carbonate is preferably at least one of dimethyl carbonate (DMC), diethyl carbonate (DEC), Ethyl Methyl Carbonate (EMC), propyl methyl carbonate (MPC), and propyl ethyl carbonate (EPC).
The lithium bis (polyfluoroalkoxy sulfonyl) imide salt is added into lithium bis (pentafluoroethyl sulfonyl) imide (Li (C)2F5SO2)2N), lithium trifluoromethylpentafluoroethylsulfonate (Li (CF)3SO2)(C2F5SO2) N), lithium bistrifluoromethylsulfonate (Li (CF)3SO2)2N) and lithium bis (fluorosulfonyl) imide (LiFSI).
The organic nitrile is at least one of succinonitrile (110-61-2), adiponitrile (111-69-3), glutaronitrile (544-13-8), 3' -oxydipropyronitrile (CAS:1656-48-0), ethylene glycol bis (propionitrile) ether (CAS:3386-87-6), 1,2, 3-tris (2-cyanato) propane (2465-93-2), 1,3, 5-pentanetrimethylnitrile (4379-04-8), 1,2, 3-propanetricyanide (62872-44-0), and 1,3, 6-hexanetrinitrile (1772-25-4).
The lithium salt is LiPF6、LiBF4、LiC1O4、LiAsF6、LiBOB，LiDFOB、LiPF4C2O4Or (ii) at least one of.
The common lithium battery electrolyte additive comprises at least one of Vinylene Carbonate (VC), vinyl sulfate (DTD), Ethylene Sulfite (ES), 1, 3-propane sultone, 1, 3-propene sultone, 1, 4-butane sultone and 1, 4-butanediol sulfate.
Example 1
Preparing electrolyte in a BRAUN glove box, filling nitrogen with the purity of 99.999% in the glove box, controlling the water content in the glove box to be less than or equal to 5ppm, and controlling the temperature at room temperature. 30 g of EC and 70 g of EMC are mixed uniformly, sealed, placed in a refrigerator to be cooled to 8 ℃, transferred into a glove box, and then LiPF is added in two batches6Fully mixing to form a non-aqueous electrolyte of a lithium ion battery with a common lithium salt molar concentration of 1mol/L, adding FEC accounting for 3 percent of the total mass of the solvent, 2 percent LIFSI, 3 percent propane sultone and 2 percent adiponitrile 1.5 into the non-aqueous electrolyte, uniformly mixing,obtaining the high-voltage lithium ion nonaqueous electrolyte.
The following preparation methods of other examples and comparative examples were carried out by referring to the preparation method of example 1.
Among them, FEC (CAS:114435-02-8), 1,3, 5-pentanitrile (4379-04-8), 1,2, 3-propanetrimethylonitrile (62872-44-0), 1,3, 6-hexanetricarbonitrile (1772-25-4), 1, 3-propanesultone (21806-61-1), 1, 3-propanesultone, 1, 8-naphthalenesulfonate (83-31-8),1, 4-butanesultone (1633-83-6), 1, 4-butanesultone (CAS:1633-83-6), methanedisulfonic acid methyl ester (CAS:99591-74-9), 1, 4-butanediol sulfate, propenyl-1, 3-sultone (CAS:21806-61-1) and other materials are available from Bailingwei science Co., Ltd, DFEC (CAS:311810-76-1), lithium bis-pentafluoroethylsulfonate (Li (C) from Suwei (Shanghai) Co., Ltd2F5SO2)2N), lithium trifluoromethylpentafluoroethylsulfonate (Li (CF)3SO2)(C2F5SO2) N), lithium bistrifluoromethylsulfonate (Li (CF)3SO2)2N), lithium bis (fluorosulfonyl) imide (LiFSI) was purchased from suzhou subfamily chemicals, inc.
Table 1: component content tables of examples 1 to 5
Table 2: component content of comparative examples 1 to 3
Performance testing
Preparing a positive plate: preparation of lithium ionPositive pole piece of the cell: dissolving 3% polyvinylidene fluoride (PVDF) in 1-methyl-9-pyrrolidone solution, and 96% lithium cobaltate (LiCoO)2) Adding 3 percent of conductive agent carbon black by mass into the solution, uniformly mixing, coating the mixed slurry on two sides of a positive current collector formed by aluminum foil, drying and pressing to obtain a positive pole piece, wherein the compaction density of the positive pole is 4.05g/cm3。
Preparing a negative pole piece: dissolving 4% by mass of SBR (polystyrene and butadiene suspension) binder and 1% by mass of CMC (sodium carboxymethylcellulose) thickener in an aqueous solution, adding 95% by mass of graphite into the solution, uniformly mixing, coating the mixed slurry on two sides of a negative current collector formed by copper foils, drying and pressing to obtain the negative pole piece.
The dry cell takes high-pressure lithium cobaltate as a positive electrode, graphite as a negative electrode and a microporous polyethylene film as a diaphragm to prepare a square dry cell. And (3) drying the dry battery cell in an oven at the temperature of 80-85 ℃ for 48 hours, and then transferring the dry battery cell into a glove box for later use. The electrolyte obtained in each of the above examples and comparative examples was injected into the dried dry cell, and then left to stand for 24 hours, and after preliminary charging, sealing and secondary formation, experimental batteries of examples and comparative examples were obtained.
High voltage 2℃ quick charge cycle performance test the experimental batteries of the examples and comparative examples were subjected to a 3-4.35V battery cycle performance test at room temperature of 25 + -2 deg.C and a relative humidity of 45-75%, the test procedure being: a.2C is charged to 4.35V by constant current, and then is charged to 0.05C by constant voltage; standing for 10 minutes; b, discharging to 3.0V at a constant current of 1C, and standing for 10 minutes; c. and (c) circulating the steps a and b for 400 times, wherein the circulation times are 300-400 times. The test results are shown in the attached Table 1.
High voltage 2℃ quick charge cycle performance test the experimental batteries of the examples and comparative examples were subjected to a 3-4.35V battery cycle performance test at room temperature of 25 + -2 deg.C and a relative humidity of 45-75%, the test procedure being:
a.2C is charged to 4.35V by constant current, and then is charged to 0.05C by constant voltage; standing for 10 minutes;
b, discharging to 3.0V at a constant current of 1C, and standing for 10 minutes;
c. and (c) circulating the steps a and b for 400 times, wherein the circulation times are 300-400 times. The test results are shown in the attached Table 1.
High-temperature storage performance test, namely performing 3-4.35V battery cycle performance test on experimental batteries of examples and comparative examples at the room temperature of 25 +/-2 ℃ and the relative humidity of 45-75%, wherein the test steps are as follows:
a.1C constant current charging to 4.35V, then constant voltage charging to cutoff current of 0.05C, and testing the thickness of the battery;
and b, transferring the battery into an incubator at 85 ℃, storing for 4H, testing the thickness of the battery after cooling, and calculating the expansion rate of the cold-test thickness.
As can be seen from the high-voltage quick-charging cycle performance test data, the high-temperature 45-degree high-voltage 2C quick-charging cycle performance test data and the high-temperature storage data at 60 ℃ for 7 days in table 2, the capacity retention rate of the battery adopting the embodiment of the non-aqueous electrolyte is more than 80% after 300 cycles, and the thickness expansion rate of the 85-degree 4H high-temperature stock is less than 5%, so that the actual use requirement of the battery is met; the capacity retention rate of the battery adopting the electrolyte in the prior art is low, and the high-temperature quick-charging performance and the normal-temperature quick-charging performance cannot be considered at the same time. The results show that when one, two or three of the positive film forming additive, the organic nitrile additive and the fluoro-carbonate additive are independently adopted, the normal-temperature quick-charging cycle performance, the high-temperature quick-charging cycle performance and the high-temperature storage performance of the battery can not meet the use requirements of people, but the combined use of the four additives can achieve the normal-temperature quick-charging cycle performance and the high-temperature quick-charging cycle performance and simultaneously has very good high-temperature storage performance.
Table 2: results of cyclic testing of examples and comparative examples
The positive electrode film-forming additive, the fluorinated ester, the organic nitrile compound and the lithium bis (polyfluoroalkoxy sulfonyl) imide used in the electrolyte of the embodiment of the invention can synergistically improve the normal-temperature and high-temperature fast charge cycle performance of the battery under voltage and can improve the high-temperature storage performance, so that the electrolyte system of the invention has high discharge capacity under higher charge and discharge voltage, and good normal-temperature and high-temperature fast charge cycle performance and high-temperature storage performance.
Compared with the prior art, the invention has the following advantages and effects:
(1) the high-voltage lithium battery prepared by using the non-aqueous electrolyte of the high-voltage lithium battery has good normal-temperature and high-temperature 2C and above rate fast-charging cycle performance.
(2) The high-voltage lithium battery prepared by using the non-aqueous electrolyte of the high-voltage lithium battery has better high-temperature storage performance.
(3) The non-aqueous electrolyte of the high-voltage lithium ion battery has relatively moderate cost.
Claims (8)
1. A non-aqueous electrolyte of a high-voltage quick-charging lithium ion battery is characterized by comprising a solvent, a common lithium salt, a positive electrode film-forming additive, a bis (polyfluoroalkoxy sulfonyl) imide lithium salt, a fluoro-ester additive and an organic nitrile additive, wherein,
the solvent is cyclic carbonate and/or chain carbonate, and the molar concentration of the common lithium salt in the solvent is 0.8-1.5 mol/L.
2. The nonaqueous electrolytic solution of claim 1, wherein the cyclic carbonate is at least one of ethylene carbonate, propylene carbonate, fluoroethylene carbonate and γ -butyrolactone.
3. The nonaqueous electrolytic solution of claim 1, wherein the chain carbonate is at least one of dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, propyl methyl carbonate, and propyl ethyl carbonate.
4. The nonaqueous electrolytic solution of claim 1, wherein the fluorocarbonate-based additive is fluoroethylene carbonate and/or difluoroethylene carbonate.
5. The nonaqueous electrolytic solution of claim 1, wherein the lithium salt of bis (polyfluoroalkoxy sulfonyl) imide is at least one of lithium bis (pentafluoroethyl sulfonate imide, lithium trifluoromethyl pentafluoroethyl sulfonate imide, lithium bis (trifluoromethyl) sulfonate imide and lithium bis (fluorosulfonyl) imide.
The nonaqueous electrolytic solution of claim 1, wherein the organic nitrile is at least one selected from succinonitrile, adiponitrile, glutaronitrile, 3' -oxydiproponitrile, ethylene glycol bis (propionitrile) ether, 1,2, 3-tris (2-cyanato) propane, 1,3, 5-pentanetrimethylnitrile, 1,2, 3-propanetricitrile, and 1,3, 6-hexanetrinitrile.
6. The nonaqueous electrolytic solution of claim 1, wherein the positive electrode film-forming additive is at least one of vinyl ethylene carbonate, methylene methanedisulfonate, tris (trimethylsilane) borate, tris (trimethylsilane) phosphate, and tris (trimethylsilane) phosphate.
7. The non-aqueous power supply of claim 1An electrolyte, characterized in that the common lithium salt is LiPF6、LiBF4、LiC1O4、LiAsF6LiBOB, LiDFOB and LiPF4C2O4At least one of (1).
8. The nonaqueous electrolytic solution of claim 1, comprising a common lithium battery electrolyte additive, wherein the common lithium battery electrolyte additive is contained in an amount of 0 to 10 parts by weight; the common lithium battery electrolyte additive is at least one of vinylene carbonate, vinyl sulfate, ethylene sulfite, 1, 3-propane sultone, 1, 3-propene sultone, 1, 4-butane sultone, 1, 4-butanediol sulfate and propenyl-1, 3-sultone.
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