CN113767502B - Nonaqueous electrolyte solution for lithium secondary battery and lithium secondary battery comprising same - Google Patents
Nonaqueous electrolyte solution for lithium secondary battery and lithium secondary battery comprising same Download PDFInfo
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- CN113767502B CN113767502B CN202080033021.7A CN202080033021A CN113767502B CN 113767502 B CN113767502 B CN 113767502B CN 202080033021 A CN202080033021 A CN 202080033021A CN 113767502 B CN113767502 B CN 113767502B
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- Prior art keywords
- electrolyte solution
- lithium secondary
- nonaqueous electrolyte
- secondary battery
- lithium
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 94
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 94
- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 68
- 239000003960 organic solvent Substances 0.000 claims abstract description 50
- 239000000654 additive Substances 0.000 claims abstract description 27
- 230000000996 additive effect Effects 0.000 claims abstract description 23
- 150000001875 compounds Chemical class 0.000 claims abstract description 21
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 15
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 15
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 22
- 229910052739 hydrogen Inorganic materials 0.000 claims description 19
- 239000001257 hydrogen Substances 0.000 claims description 19
- 239000002184 metal Substances 0.000 claims description 17
- 229910052751 metal Inorganic materials 0.000 claims description 15
- 125000000217 alkyl group Chemical group 0.000 claims description 13
- 125000004432 carbon atom Chemical group C* 0.000 claims description 13
- 150000002431 hydrogen Chemical class 0.000 claims description 13
- 239000007774 positive electrode material Substances 0.000 claims description 11
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 9
- 239000011572 manganese Substances 0.000 claims description 8
- 229910052782 aluminium Inorganic materials 0.000 claims description 7
- 229910052759 nickel Inorganic materials 0.000 claims description 7
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 3
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 3
- 229910052748 manganese Inorganic materials 0.000 claims description 3
- 229910017052 cobalt Inorganic materials 0.000 claims description 2
- 239000010941 cobalt Substances 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- 230000001976 improved effect Effects 0.000 abstract description 7
- 229940021013 electrolyte solution Drugs 0.000 description 79
- 230000000052 comparative effect Effects 0.000 description 30
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 25
- 125000004093 cyano group Chemical group *C#N 0.000 description 22
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- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 12
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 6
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- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 4
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- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 238000009831 deintercalation Methods 0.000 description 3
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- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 description 3
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- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 description 2
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
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- 101150058243 Lipf gene Proteins 0.000 description 2
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- SOXUFMZTHZXOGC-UHFFFAOYSA-N [Li].[Mn].[Co].[Ni] Chemical compound [Li].[Mn].[Co].[Ni] SOXUFMZTHZXOGC-UHFFFAOYSA-N 0.000 description 1
- ZYXUQEDFWHDILZ-UHFFFAOYSA-N [Ni].[Mn].[Li] Chemical compound [Ni].[Mn].[Li] ZYXUQEDFWHDILZ-UHFFFAOYSA-N 0.000 description 1
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 description 1
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
- 230000001070 adhesive effect Effects 0.000 description 1
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 description 1
- 150000001408 amides Chemical class 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 1
- LJCFOYOSGPHIOO-UHFFFAOYSA-N antimony pentoxide Inorganic materials O=[Sb](=O)O[Sb](=O)=O LJCFOYOSGPHIOO-UHFFFAOYSA-N 0.000 description 1
- 229910000411 antimony tetroxide Inorganic materials 0.000 description 1
- GHPGOEFPKIHBNM-UHFFFAOYSA-N antimony(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Sb+3].[Sb+3] GHPGOEFPKIHBNM-UHFFFAOYSA-N 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- RQNWIZPPADIBDY-UHFFFAOYSA-N arsenic atom Chemical compound [As] RQNWIZPPADIBDY-UHFFFAOYSA-N 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- 229910052790 beryllium Inorganic materials 0.000 description 1
- ATBAMAFKBVZNFJ-UHFFFAOYSA-N beryllium atom Chemical compound [Be] ATBAMAFKBVZNFJ-UHFFFAOYSA-N 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 1
- 229910000417 bismuth pentoxide Inorganic materials 0.000 description 1
- IAQRGUVFOMOMEM-UHFFFAOYSA-N butene Natural products CC=CC IAQRGUVFOMOMEM-UHFFFAOYSA-N 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- SIXOAUAWLZKQKX-UHFFFAOYSA-N carbonic acid;prop-1-ene Chemical compound CC=C.OC(O)=O SIXOAUAWLZKQKX-UHFFFAOYSA-N 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003610 charcoal Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 229910001914 chlorine tetroxide Inorganic materials 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- CKFRRHLHAJZIIN-UHFFFAOYSA-N cobalt lithium Chemical compound [Li].[Co] CKFRRHLHAJZIIN-UHFFFAOYSA-N 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 229940093499 ethyl acetate Drugs 0.000 description 1
- CYEDOLFRAIXARV-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound CCCOC(=O)OCC CYEDOLFRAIXARV-UHFFFAOYSA-N 0.000 description 1
- 239000011326 fired coke Substances 0.000 description 1
- 239000006260 foam Substances 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 229910052730 francium Inorganic materials 0.000 description 1
- KLMCZVJOEAUDNE-UHFFFAOYSA-N francium atom Chemical compound [Fr] KLMCZVJOEAUDNE-UHFFFAOYSA-N 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 229910052735 hafnium Inorganic materials 0.000 description 1
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- 229920001519 homopolymer Polymers 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 238000001453 impedance spectrum Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- 230000001939 inductive effect Effects 0.000 description 1
- 229910001387 inorganic aluminate Inorganic materials 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- YADSGOSSYOOKMP-UHFFFAOYSA-N lead dioxide Inorganic materials O=[Pb]=O YADSGOSSYOOKMP-UHFFFAOYSA-N 0.000 description 1
- XMFOQHDPRMAJNU-UHFFFAOYSA-N lead(II,IV) oxide Inorganic materials O1[Pb]O[Pb]11O[Pb]O1 XMFOQHDPRMAJNU-UHFFFAOYSA-N 0.000 description 1
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 1
- 229910001547 lithium hexafluoroantimonate(V) Inorganic materials 0.000 description 1
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 description 1
- RSNHXDVSISOZOB-UHFFFAOYSA-N lithium nickel Chemical compound [Li].[Ni] RSNHXDVSISOZOB-UHFFFAOYSA-N 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 229910001537 lithium tetrachloroaluminate Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- 229910000686 lithium vanadium oxide Inorganic materials 0.000 description 1
- HSFDLPWPRRSVSM-UHFFFAOYSA-M lithium;2,2,2-trifluoroacetate Chemical compound [Li+].[O-]C(=O)C(F)(F)F HSFDLPWPRRSVSM-UHFFFAOYSA-M 0.000 description 1
- VGYDTVNNDKLMHX-UHFFFAOYSA-N lithium;manganese;nickel;oxocobalt Chemical compound [Li].[Mn].[Ni].[Co]=O VGYDTVNNDKLMHX-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 239000006051 mesophase pitch carbide Substances 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- QPJSUIGXIBEQAC-UHFFFAOYSA-N n-(2,4-dichloro-5-propan-2-yloxyphenyl)acetamide Chemical compound CC(C)OC1=CC(NC(C)=O)=C(Cl)C=C1Cl QPJSUIGXIBEQAC-UHFFFAOYSA-N 0.000 description 1
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 1
- KTQDYGVEEFGIIL-UHFFFAOYSA-N n-fluorosulfonylsulfamoyl fluoride Chemical compound FS(=O)(=O)NS(F)(=O)=O KTQDYGVEEFGIIL-UHFFFAOYSA-N 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- 239000011356 non-aqueous organic solvent Substances 0.000 description 1
- 229910052762 osmium Inorganic materials 0.000 description 1
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- VLTRZXGMWDSKGL-UHFFFAOYSA-M perchlorate Chemical compound [O-]Cl(=O)(=O)=O VLTRZXGMWDSKGL-UHFFFAOYSA-M 0.000 description 1
- 230000000737 periodic effect Effects 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 229910052699 polonium Inorganic materials 0.000 description 1
- HZEBHPIOVYHPMT-UHFFFAOYSA-N polonium atom Chemical compound [Po] HZEBHPIOVYHPMT-UHFFFAOYSA-N 0.000 description 1
- 229920000139 polyethylene terephthalate Polymers 0.000 description 1
- 239000005020 polyethylene terephthalate Substances 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920006389 polyphenyl polymer Polymers 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 229940090181 propyl acetate Drugs 0.000 description 1
- 229920001384 propylene homopolymer Polymers 0.000 description 1
- 229910052705 radium Inorganic materials 0.000 description 1
- HCWPIIXVSYCSAN-UHFFFAOYSA-N radium atom Chemical compound [Ra] HCWPIIXVSYCSAN-UHFFFAOYSA-N 0.000 description 1
- 238000006479 redox reaction Methods 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 229910052702 rhenium Inorganic materials 0.000 description 1
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 229910052701 rubidium Inorganic materials 0.000 description 1
- IGLNJRXAVVLDKE-UHFFFAOYSA-N rubidium atom Chemical compound [Rb] IGLNJRXAVVLDKE-UHFFFAOYSA-N 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 229910052706 scandium Inorganic materials 0.000 description 1
- SIXSYDAISGFNSX-UHFFFAOYSA-N scandium atom Chemical compound [Sc] SIXSYDAISGFNSX-UHFFFAOYSA-N 0.000 description 1
- VSZWPYCFIRKVQL-UHFFFAOYSA-N selanylidenegallium;selenium Chemical compound [Se].[Se]=[Ga].[Se]=[Ga] VSZWPYCFIRKVQL-UHFFFAOYSA-N 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 230000003746 surface roughness Effects 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 229910052713 technetium Inorganic materials 0.000 description 1
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- PAPBSGBWRJIAAV-UHFFFAOYSA-N ε-Caprolactone Chemical compound O=C1CCCCCO1 PAPBSGBWRJIAAV-UHFFFAOYSA-N 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
-
- 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
- H01M2220/00—Batteries for particular applications
- H01M2220/10—Batteries in stationary systems, e.g. emergency power source in plant
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Secondary Cells (AREA)
Abstract
The present invention relates to a nonaqueous electrolyte solution for a lithium secondary battery and a lithium secondary battery comprising the same, and in particular, an object of the present invention is to provide a nonaqueous electrolyte solution for a lithium secondary battery and a lithium secondary battery comprising a lithium salt, an organic solvent, and a compound represented by formula 1 as an additive, wherein high-rate charge-discharge characteristics at high temperature are improved by comprising the nonaqueous electrolyte solution.
Description
Technical Field
Cross Reference to Related Applications
The present application claims priority from korean patent application No. 10-2019-0147431 filed on 11.18 and korean patent application No. 10-2020-0151165 filed on 11.12 2020, the disclosures of which are incorporated herein by reference. The present application relates to a nonaqueous electrolyte solution for a lithium secondary battery and a lithium secondary battery comprising the same.
Background
The dependence of modern society on electric energy is gradually increased, and accordingly, the production of electric energy is further increased. In order to solve the environmental problems occurring in this process, renewable energy power generation is attracting attention as a next generation power generation system. For renewable energy sources, a large-capacity energy storage device is essential for stable power supply because of its intermittent power generation characteristics. Lithium ion batteries are receiving a great deal of attention as devices currently commercialized in energy storage devices that exhibit the highest energy density.
The lithium ion battery is composed of the following components: a positive electrode formed of a transition metal oxide containing lithium, a negative electrode capable of storing lithium, an electrolyte solution containing an organic solvent containing a lithium salt, and a separator.
With respect to the positive electrode in these elements, energy is stored by the redox reaction of the transition metal, wherein this results in that the transition metal must be substantially contained in the positive electrode material.
When the positive electrode active material undergoes structural collapse during repeated charge and discharge, the positive electrode performance is reduced. That is, metal ions that have been dissolved from the surface of the positive electrode during collapse of the positive electrode structure are electrodeposited on the negative electrode, thereby degrading the performance of the battery. This phenomenon is further increased when the potential of the positive electrode increases or the battery is exposed to high temperatures.
Therefore, in order to control the deterioration behavior of the battery, studies have been made to apply a film-forming additive to the positive electrode, and further, studies have been made to suppress the occurrence of electrodeposition or ion substitution of dissolved transition metal on the negative electrode.
Disclosure of Invention
Technical problem
An aspect of the present invention provides a nonaqueous electrolyte solution for a lithium secondary battery, which includes an additive that forms a complex with a transition metal ion dissolved from a positive electrode.
Another aspect of the present invention provides a lithium secondary battery in which high-rate charge-discharge characteristics are improved by including a nonaqueous electrolyte solution for a lithium secondary battery.
Technical proposal
In accordance with one aspect of the present invention,
Provided is a nonaqueous electrolyte solution for a lithium secondary battery, which contains a lithium salt, an organic solvent, and a compound represented by formula 1 as an additive.
[ 1]
Wherein, in the formula 1,
R 1 to R 6 are each independently hydrogen, an alkyl group having 1 to 5 carbon atoms or a-CN group, wherein at least one of R 1 to R 6 is a-CN group.
In accordance with another aspect of the present invention,
There is provided a lithium secondary battery comprising a negative electrode, a positive electrode, a separator provided between the negative electrode and the positive electrode, and a nonaqueous electrolyte solution, wherein the nonaqueous electrolyte solution comprises the nonaqueous electrolyte solution for a lithium secondary battery of the present invention.
Advantageous effects
The compound represented by formula 1 contained in the nonaqueous electrolyte solution of the present invention is a compound having a cyano group in its structure, wherein the cyano group can inhibit electrodeposition of metal ions on the negative electrode by forming a complex with a transition metal ion dissolved from the positive electrode of the lithium secondary battery. Since the nonaqueous electrolyte solution containing such an additive undergoes oxidative decomposition before the organic solvent to form a film on the surface of the positive electrode, it can suppress the continuous decomposition reaction between the positive electrode and the organic solvent. Accordingly, if the nonaqueous electrolyte solution is contained, a lithium secondary battery having improved high-rate charge-discharge characteristics can be realized.
Drawings
The following drawings accompanying the specification illustrate preferred embodiments of the present invention by way of example and serve to enable a further understanding of the technical concepts of the present invention together with the detailed description of the invention given below, and therefore the present invention should not be construed solely by the matters in these drawings.
Fig. 1 is a graph showing the results of electrochemical stability evaluation of a nonaqueous electrolyte solution in experimental example 1;
fig. 2 is a graph showing the results of measurement of the decomposition initiation voltage of the nonaqueous electrolyte solutions of example 3 and comparative example 2 in experimental example 2;
Fig. 3 is a graph showing differential capacitance curves of lithium secondary batteries of example 5 and comparative example 3 in experimental example 3;
fig. 4 is a graph showing the impedance evaluation results of the lithium secondary batteries of example 5 and comparative example 3 in experimental example 5; and
Fig. 5 is a graph showing the results of evaluation of the high temperature cycle characteristics of the secondary batteries of example 5 and comparative example 3 in experimental example 6.
Detailed Description
Hereinafter, the present invention will be described in more detail.
It should be understood that words or terms used in the specification and claims should not be construed as meanings defined in commonly used dictionaries, and it should be further understood that words or terms should be interpreted as having meanings consistent with their meanings in the context of the relevant art and the technical ideas of the present invention based on the principle that the inventors can properly define the words or terms to best explain the invention.
Conventionally, an acid (for example, hydrofluoric acid (HF)) formed by hydrolysis/thermal decomposition of an acid or a lithium salt generated by a side reaction between a positive electrode and an electrolyte solution, or a change in the structure of the positive electrode occurs due to repeated charge and discharge, so that a transition metal constituting the positive electrode is easily dissolved into the electrolyte solution, and dissolved transition metal ions are redeposited on the positive electrode, resulting in an increase in the resistance of the positive electrode. In addition, since a transition metal, which moves to the anode through an electrolyte solution, is electrodeposited on the anode, thereby self-discharging the anode and breaking a Solid Electrolyte Interface (SEI) that provides the anode with passivation capability, the interfacial resistance of the anode is increased by promoting an additional electrolyte solution decomposition reaction.
Since this series of reactions reduces the amount of lithium ions available in the battery, it not only results in a decrease in the capacity of the battery, but also accompanies the decomposition reaction of the electrolyte solution, thus also increasing the resistance. In addition, in the case where metal impurities are contained in the electrode when the positive electrode is disposed, since the metal impurities are dissolved from the positive electrode during initial charging, dissolved metal ions are electrodeposited on the surface of the negative electrode. The electrodeposited metal ions grow as dendrites to cause internal short circuits in the battery, and thus become a main cause of low voltage failure.
The present invention is directed to a nonaqueous electrolyte solution for a lithium secondary battery, which can form a firm film on the surface of a positive electrode through oxidative decomposition before an organic solvent by containing an additive capable of preventing electrodeposition of metal ions on the negative electrode through formation of a complex with dissolved metal ions (the cause of the above-mentioned deterioration and failure behavior), and a lithium secondary battery, in which high-rate charge and discharge at high temperature are improved by containing the nonaqueous electrolyte solution.
Nonaqueous electrolyte solution for lithium secondary battery
Specifically, in an embodiment of the present invention, there is provided a nonaqueous electrolyte solution for a lithium secondary battery, the nonaqueous electrolyte solution comprising:
a lithium salt, an organic solvent and a compound represented by formula 1 as an additive,
[ 1]
In the formula (1) of the present invention,
R 1 to R 6 are each independently hydrogen, an alkyl group having 1 to 5 carbon atoms or a-CN group, wherein at least one of R 1 to R 6 is a-CN group.
Lithium salt
First, in the nonaqueous electrolyte solution for a lithium secondary battery of the present invention, any lithium salt commonly used in the electrolyte solution for a lithium secondary battery may be used as the lithium salt without limitation, for example, the lithium salt may contain Li + as a cation and at least one selected from the group consisting of F-、Cl-、Br-、I-、NO3 -、N(CN)2 -、BF4 -、ClO4 -、B10Cl10 -、AlCl4 -、AlO4 -、PF6 -、CF3SO3 -、CH3CO2 -、CF3CO2 -、AsF6 -、SbF6 -、CH3SO3 -、(CF3CF2SO2)2N-、(CF3SO2)2N-、(FSO2)2N-、BF2C2O4 -、BC4O8 -、PF4C2O4 -、PF2C4O8 -、(CF3)2PF4 -、(CF3)3PF3 -、(CF3)4PF2 -、(CF3)5PF-、(CF3)6P-、C4F9SO3 -、CF3CF2SO3 -、CF3CF2(CF3)2CO-、(CF3SO2)2CH-、CF3(CF2)7SO3 - and SCN - as an anion.
Specifically, the lithium salt may include a single material selected from the group consisting of LiCl、LiBr、LiI、LiBF4、LiClO4、LiB10Cl10、LiAlCl4、LiAlO4、LiPF6、LiCF3SO3、LiCH3CO2、LiCF3CO2、LiAsF6、LiSbF6、LiCH3SO3、LiFSI( bis (fluorosulfonyl) imide lithium, liN (SO 2F)2), liBETI (bis (perfluoroethanesulfonyl) imide lithium, liN (SO 2CF2CF3)2) and LiTFSI (bis (trifluoromethanesulfonyl) imide lithium), liN (SO 2CF3)2), or a mixture of two or more thereof.
The lithium salt may be appropriately changed within a normal usable range, but may be contained in the electrolyte solution at a concentration of 0.8M to 4.0M (e.g., 1.0M to 3.0M) to obtain an optimal effect of forming a film for preventing corrosion of the electrode surface. If the concentration of the lithium salt is less than 0.8M, the effect of improving the low temperature output and the cycle characteristics during high temperature storage of the lithium secondary battery is insignificant, and if the concentration of the lithium salt is greater than 4.0M, the permeability of the electrolyte solution may be reduced due to the increase in the viscosity of the nonaqueous electrolyte solution.
(2) Organic solvents
In the nonaqueous electrolyte solution for a lithium secondary battery of the present specification, the organic solvent may include a cyclic carbonate-based organic solvent, a linear carbonate-based organic solvent, or a mixed organic solvent thereof.
The cyclic carbonate-based organic solvent is an organic solvent that can well dissociate lithium salts in the electrolyte due to a high dielectric constant as a high-viscosity organic solvent, wherein specific examples of the cyclic carbonate-based organic solvent may be at least one organic solvent selected from the group consisting of Ethylene Carbonate (EC), propylene Carbonate (PC), 1, 2-butylene carbonate, 2, 3-butylene carbonate, 1, 2-pentylene carbonate, 2, 3-pentylene carbonate, and vinylene carbonate, wherein the cyclic carbonate-based organic solvent may include ethylene carbonate.
Further, the linear carbonate-based organic solvent is an organic solvent having a low viscosity and a low dielectric constant, wherein a typical example of the linear carbonate-based organic solvent may be at least one organic solvent selected from the group consisting of dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate, ethyl Methyl Carbonate (EMC), methyl propyl carbonate and ethyl propyl carbonate, and the linear carbonate-based organic solvent may specifically include Ethyl Methyl Carbonate (EMC).
In order to prepare an electrolyte solution having high ionic conductivity, a mixed organic solvent of a cyclic carbonate-based organic solvent and a linear carbonate-based organic solvent may be used as the organic solvent.
In addition, the organic solvent may include a linear ester-based organic solvent and/or a cyclic ester-based organic solvent in addition to the cyclic carbonate-based organic solvent and/or the linear carbonate-based organic solvent.
Specific examples of the linear ester-based organic solvent may be at least one organic solvent selected from the group consisting of methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, propyl propionate, and butyl propionate.
In addition, the cyclic carbonate-based organic solvent may include at least one organic solvent selected from the group consisting of gamma-butyrolactone, gamma-valerolactone, gamma-caprolactone, sigma-valerolactone and epsilon-caprolactone.
If necessary, the organic solvent may be used by being added to an organic solvent commonly used in an electrolyte solution for a lithium secondary battery, without limitation. For example, the organic solvent may further include at least one selected from the group consisting of an ether-based organic solvent, an amide-based organic solvent, and a nitrile-based organic solvent.
(3) Additive agent
The nonaqueous electrolyte solution for lithium secondary batteries of the present invention may contain a compound represented by the following formula 1 as an additive.
[ 1]
In the formula (1) of the present invention,
R 1 to R 6 are each independently hydrogen, an alkyl group having 1 to 5 carbon atoms or a-CN group, wherein at least one of R 1 to R 6 is a-CN group.
Specifically, in formula 1, R 1 to R 6 may each independently be hydrogen, an alkyl group having 1 to 4 carbon atoms, or a-CN group, wherein at least one of R 1 to R 6 may be a-CN group.
Further, in formula 1, R 1 may be an alkyl group having 1 to 3 carbon atoms or a-CN group, R 2 may be hydrogen or an alkyl group having 1 to 3 carbon atoms, R 3 to R 6 may each independently be hydrogen, an alkyl group having 1 to 4 carbon atoms, or a-CN group, wherein at least one of R 1、R3 to R 6 may be a-CN group.
Further, in formula 1, R 1 may be a-CN group, R 2 may be hydrogen or an alkyl group having 1 to 3 carbon atoms, and R 3 to R 6 may each independently be hydrogen, an alkyl group having 1 to 3 carbon atoms, or a-CN group.
Further, in formula 1, R 1 may be a-CN group, R 2 may be hydrogen, R 3 and R 6 may each independently be hydrogen or a-CN group, and R 4 and R 5 may each independently be hydrogen, an alkyl group having 1 to 3 carbon atoms, or a-CN group.
Further, in formula 1, R 1 may be a-CN group, R 2 may be hydrogen, R 3 and R 6 may each independently be hydrogen, and R 4 and R 5 may each independently be hydrogen or a-CN group.
Preferably, the compound represented by formula 1 may be a compound represented by the following formula 1a, for example, coumarin-3-carbonitrile.
[ 1A ]
In the present invention, the compound represented by formula 1 contained as an electrolyte solution additive is a compound having a cyano group in its structure, wherein the cyano group can inhibit electrodeposition of metal ions on the negative electrode by forming a complex with the metal ions dissolved from the positive electrode of the lithium secondary battery. In addition, the additive can form a firm film on the surface of the positive electrode by oxidative decomposition before the organic solvent, and the film can suppress continuous decomposition reaction between the positive electrode and the organic solvent. Therefore, a lithium secondary battery having improved high-rate charge and discharge can be realized by including a nonaqueous electrolyte solution (including an additive).
The content of the compound of formula 1 may be 0.05 wt% or more and less than 1.2 wt%, for example, 0.1 wt% to 1 wt%, based on the total weight of the nonaqueous electrolyte solution.
In the case where the content of the compound represented by formula 1 is within the above-described range, a secondary battery having more improved overall performance can be produced. For example, in the case where the content of the compound represented by formula 1 is 0.05 wt% or more and less than 1.2 wt%, it can remove metal ions and complexes and can simultaneously form a strong film on the surface of the positive electrode while suppressing as much as possible drawbacks such as side reactions caused by additives, decrease in initial capacity, and increase in resistance. If the content of the compound represented by formula 1 is 1.2 wt% or more, side reactions due to the additives may occur or an initial capacity decrease due to an increase in resistance may occur due to a decrease in solubility of the additives in the nonaqueous organic solvent.
Lithium secondary battery
Further, in another embodiment of the present invention, there is provided a lithium secondary battery comprising the nonaqueous electrolyte solution for a lithium secondary battery of the present invention.
The lithium secondary battery of the present invention may be prepared as follows: an electrode assembly in which a positive electrode, a negative electrode, and a separator disposed between the positive electrode and the negative electrode are sequentially stacked, the electrode assembly is contained in a battery case, and then the nonaqueous electrolyte solution of the present invention is injected.
As a method for preparing the lithium secondary battery of the present invention, typical methods known in the art may be used, and specifically, the method for preparing the lithium secondary battery of the present invention is as follows.
(1) Positive electrode
The positive electrode may be prepared by coating a positive electrode current collector with a positive electrode slurry including a positive electrode active material, a binder, a conductive agent, and a solvent, and then drying and roll-pressing the coated positive electrode current collector.
The positive electrode current collector is not particularly limited as long as it has conductivity without causing adverse chemical changes in the battery, and for example, stainless steel, aluminum, nickel, titanium, fired carbon, or aluminum or stainless steel surface-treated with one of carbon, nickel, titanium, silver, or the like may be used.
The positive electrode active material is a compound capable of reversibly intercalating and deintercalating lithium, wherein the positive electrode active material may specifically include a lithium composite metal oxide including lithium and at least one metal selected from the group consisting of nickel (Ni), cobalt (Co), manganese (Mn), iron (Fe), and aluminum (Al).
More specifically, the lithium composite metal oxide may include: lithium-manganese-based oxides (e.g., liMnO 2、LiMn2O4, etc.), lithium-cobalt-based oxides (e.g., liCoO 2, etc.), lithium-nickel-based oxides (e.g., liNiO 2, etc.), lithium-nickel-manganese-based oxides (e.g., liNi 1-YMnYO2 (where 0< y < 1), liMn 2-ZNiZO4 (where 0< z < 2)), lithium-nickel-cobalt-based oxides (e.g., liNi 1-Y1CoY1O2 (where 0< y1< 1)) Lithium-manganese-cobalt-based oxides (e.g., liCo 1-Y2MnY2O2 (where 0< y2< 1), liMn 2-Z1CoZ1O4 (where 0< z1< 2)), lithium-nickel-manganese-cobalt-based oxides (e.g., li (Ni pCoqMnr1)O2 (where 0< p <1, 0< q <1, 0< r1<1, and p+q+r1=1) or Li (Ni p1Coq1Mnr2)O4 (where 0< p1<2, 0< q1<2, 0< r2, and p1+q1+r2=2), Or lithium-nickel-cobalt-transition metal (M) oxide (e.g., li (Ni p2Coq2Mnr3MS2)O2 (where M is selected from the group consisting of aluminum (Al), iron (Fe), vanadium (V), chromium (Cr), titanium (Ti), tantalum (Ta), magnesium (Mg), and molybdenum (Mo), and p2, q2, r3, and S2 are the atomic fractions of each individual element, where 0< p2<1, 0< q2<1, 0< r3<1, 0< S2<1, and p2+q2+r3+s2=1), may include any one or two or more compounds thereof. Among these materials, in terms of improving capacity characteristics and stability of the battery, the lithium composite metal oxide may include LiCoO 2、LiMnO2、LiNiO2, lithium nickel manganese cobalt oxide (e.g., li (Ni 0.6Mn0.2Co0.2)O2、Li(Ni0.5Mn0.3Co0.2)O2 or Li (Ni 0.8Mn0.1Co0.1)O2), or lithium nickel cobalt aluminum oxide (e.g., liNi 0.8Co0.15Al0.05O2, etc.), and the lithium composite metal oxide may include Li(Ni0.6Mn0.2Co0.2)O2、Li(Ni0.5Mn0.3Co0.2)O2、Li(Ni0.7Mn0.15Co0.15)O2、 or Li (Ni 0.8Mn0.1Co0.1)O2, any one of which or a mixture of two or more thereof may be used) in view of significant improvement by controlling the type and content ratio of elements constituting the lithium composite metal oxide.
The content of the positive electrode active material may be 80 to 99 wt%, for example, 90 to 99 wt%, based on the total weight of the solids in the positive electrode slurry. When the amount of the positive electrode active material is 80 wt% or less, the capacity decreases due to a decrease in energy density.
The binder is a component that contributes to adhesion between the active material and the conductive agent and adhesion to the current collector, wherein the binder is generally added in an amount of 1 to 30% by weight based on the total weight of solids in the positive electrode slurry. Examples of binders may be polyvinylidene fluoride, polyvinyl alcohol, carboxymethyl cellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, polyvinylpyrrolidone, polytetrafluoroethylene, polyethylene, polypropylene, styrene-butadiene rubber, fluororubber, various copolymers, and the like.
Further, the conductive agent is a material that provides conductivity without causing adverse chemical changes in the battery, wherein the conductive agent may be added in an amount of 1 to 20% by weight based on the total weight of solids in the positive electrode slurry.
As typical examples of the conductive agent, the following conductive materials may be used, for example: carbon powder such as carbon black, acetylene black, ketjen black, channel black, furnace black, lamp black or thermal black; graphite powder such as natural graphite, artificial graphite or graphite having a developed crystal structure; conductive fibers such as carbon fibers or metal fibers; conductive powders such as fluorocarbon powder, aluminum powder, and nickel powder; conductive whiskers such as zinc oxide whiskers and potassium titanate whiskers; conductive metal oxides such as titanium oxide; or a polyphenylene derivative.
In addition, the solvent may include an organic solvent, such as N-methyl-2-pyrrolidone (NMP), and may be used in an amount such that a desired viscosity is obtained when the positive electrode active material, and optionally, a binder and a conductive agent are included. For example, the content of the solvent may be such that the concentration of solids in the slurry including the positive electrode active material and optionally the binder and the conductive agent is in the range of 10 to 60 wt%, for example, 20 to 50 wt%.
(2) Negative electrode
The anode may be prepared by coating an anode current collector with an anode slurry including an anode active material, a binder, a conductive agent, and a solvent, and then drying and roll-pressing the coated anode current collector.
The negative electrode current collector generally has a thickness of 3 μm to 500 μm. The anode current collector is not particularly limited as long as it has high conductivity without causing adverse chemical changes in the battery, for example, copper, stainless steel, aluminum, nickel, titanium, fired carbon; copper or stainless steel surface-treated with one of carbon, nickel, titanium, silver, etc.; aluminum-cadmium alloys, and the like. Further, the anode current collector may have fine surface roughness to improve the adhesive strength with the anode active material, similarly to the cathode current collector, and the anode current collector may be used in various shapes such as a film, a sheet, a foil, a net, a porous body, a foam, a non-woven fabric body, and the like.
In addition, the anode active material may include at least one selected from the group consisting of metallic lithium, a carbon material capable of reversibly intercalating/deintercalating lithium ions, a metal or an alloy of lithium and a metal, a metal composite oxide, a material that can be doped and undoped with lithium, and a transition metal oxide.
As the carbon material capable of reversibly intercalating/deintercalating lithium ions, a carbon-based anode active material commonly used in lithium ion secondary batteries may be used without particular limitation, and as a typical example, crystalline carbon, amorphous carbon, or both thereof may be used. Examples of crystalline carbon may be graphite, such as natural graphite or artificial graphite in an irregular, planar, flaky, spherical or fibrous form, and examples of amorphous carbon may be soft carbon (low-temperature sintered carbon) or hard carbon, mesophase pitch carbide and fired coke.
As the metal or the alloy of lithium and metal, a metal selected from the group consisting of copper (Cu), nickel (Ni), sodium (Na), potassium (K), rubidium (Rb), cesium (Cs), francium (Fr), beryllium (Be), magnesium (Mg), calcium (Ca), strontium (Sr), silicon (Si), antimony (Sb), lead (Pb), indium (In), zinc (Zn), barium (Ba), radium (Ra), germanium (Ge), aluminum (Al), and tin (Sn), or an alloy of lithium and metal can Be used.
One selected from the group consisting of PbO、PbO2、Pb2O3、Pb3O4、Sb2O3、Sb2O4、Sb2O5、GeO、GeO2、Bi2O3、Bi2O4、Bi2O5、LixFe2O3(0≤x≤1)、LixWO2(0≤x≤1) and Sn xMe1-xMe'yOz (Me: manganese (Mn), fe, pb or Ge; me': al, boron (B), phosphorus (P), si, group I, II of the periodic Table of the elements and group III elements or halogens; 0< x.ltoreq.1; 1.ltoreq.y.ltoreq.3; 1.ltoreq.z.ltoreq.8) may be used as the metal composite oxide.
The materials that can be doped and undoped with lithium may include Si, siO x (0 < x.ltoreq.2), si-Y alloys (where Y is an element selected from the group consisting of alkali metals, alkaline earth metals, group 13 elements, group 14 elements, transition metals, rare earth elements, and combinations thereof, and is not Si), sn, snO 2, and Sn-Y (where Y is an element selected from the group consisting of alkali metals, alkaline earth metals, group 13 elements, group 14 elements, transition metals, rare earth elements, and combinations thereof, and is not Sn), and mixtures of SiO 2 and at least one thereof may also be used. The element Y may be selected from Mg, ca, sr, ba, ra, scandium (Sc), yttrium (Y), ti, zirconium (Zr), hafnium (Hf),(Rf), V, niobium (Nb), ta,/>(Db), cr, mo, tungsten (W),/>(Sg), technetium (Tc), rhenium (Re),/>(Bh), fe, pb, ruthenium (Ru), osmium (Os),/>(Hs), rhodium (Rh), iridium (Ir), palladium (Pd), platinum (Pt), cu, silver (Ag), gold (Au), zn, cadmium (Cd), B, al, gallium (Ga), sn, in, ge, P, arsenic (As), sb, bismuth (Bi), sulfur (S), selenium (Se), tellurium (Te), polonium (Po) and combinations thereof.
The transition metal oxide may include lithium-containing titanium composite oxide (LTO), vanadium oxide, and lithium vanadium oxide.
The content of the anode active material may be 80 to 99 wt% based on the total weight of solids in the anode slurry.
The binder is a component that contributes to adhesion between the conductive agent, the active material, and the current collector, wherein the binder is generally added in an amount of 1 to 30% by weight based on the total weight of solids in the anode slurry. Examples of binders may be polyvinylidene fluoride, polyvinyl alcohol, carboxymethyl cellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, polyvinylpyrrolidone, polytetrafluoroethylene, polyethylene, polypropylene, styrene-butadiene rubber, fluororubber and various copolymers thereof.
The conductive agent is a component for further improving the conductivity of the anode active material, wherein the conductive agent may be added in an amount of 1 to 20 wt% based on the total weight of solids in the anode slurry. Any conductive agent may be used without particular limitation as long as it has conductivity without inducing adverse chemical changes in the battery, for example, the following conductive materials may be used, for example: carbon powder such as carbon black, acetylene black, ketjen black, channel black, furnace black, lamp black or thermal black; graphite powder such as natural graphite, artificial graphite or graphite having a developed crystal structure; conductive fibers such as carbon fibers or metal fibers; conductive powders such as fluorocarbon powder, aluminum powder, and nickel powder; conductive whiskers such as zinc oxide whiskers and potassium titanate whiskers; conductive metal oxides such as titanium oxide; or a polyphenyl derivative.
The solvent may include water or an organic solvent such as NMP and alcohol, and the solvent may be used in such an amount that a desired viscosity is obtained when the anode active material, and optionally, a binder and a conductive agent are included. For example, the content of the solvent may be such that the concentration of solids in the anode slurry including the anode active material and optionally the binder and the conductive agent is in the range of 50 to 75 wt%, for example, 50 to 65 wt%.
(3) Diaphragm
A typical porous polymer film that is generally used, for example, a porous polymer film prepared from a polyolefin-based polymer (e.g., an ethylene homopolymer, a propylene homopolymer, an ethylene/butene copolymer, an ethylene/hexene copolymer, and an ethylene/methacrylate copolymer) may be used alone or in a laminate, and as a separator included in the lithium secondary battery of the present invention, a typical porous non-woven fabric, for example, a non-woven fabric formed of a high-melting glass fiber or a polyethylene terephthalate fiber, may be used, but the present invention is not limited thereto.
The shape of the lithium secondary battery of the present invention is not particularly limited, and a cylindrical, prismatic, pouch or coin type using a can may be used.
Hereinafter, the present invention will be described in more detail according to examples. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these example embodiments are provided so that this description will be thorough and complete, and will fully convey the scope of the invention to those skilled in the art.
Examples
I. preparation of nonaqueous electrolyte solution for lithium secondary battery
Comparative example 1
After Ethylene Carbonate (EC) and methyl ethylene carbonate (EMC) were mixed at a volume ratio of 1:2, liPF 6 was dissolved so that the concentration of LiPF 6 was 1.0M, thereby preparing an electrolyte solution (a-1).
Comparative example 2
After Ethylene Carbonate (EC), propylene Carbonate (PC), ethyl Propionate (EP), and Propyl Propionate (PP) were mixed at a volume ratio of 2:1:2.5:4.5, liPF 6 and LiFSI were dissolved so that the concentrations of LiPF 6 and LiFSI were 0.8M and 0.2M, respectively, to prepare an electrolyte solution (a-2).
Example 1
The nonaqueous electrolyte solution (B-1) for a lithium secondary battery of the present invention was prepared by adding 0.1g of coumarin-3-carbonitrile to 99.9g of the electrolyte solution (A-1) of comparative example 1.
Example 2
The nonaqueous electrolyte solution (B-2) for a lithium secondary battery of the present invention was prepared by adding 1.0g of coumarin-3-carbonitrile to 99.0g of the electrolyte solution (A-1) of comparative example 1.
Example 3
The nonaqueous electrolyte solution (B-3) for a lithium secondary battery of the present invention was prepared by adding 0.2g of coumarin-3-carbonitrile to 99.8g of the electrolyte solution (A-2) of comparative example 2.
Example 4
The nonaqueous electrolyte solution (B-4) for a lithium secondary battery of the present invention was prepared by adding 1.2g of coumarin-3-carbonitrile to 98.8g of the electrolyte solution (A-2) of comparative example 2.
II preparation of secondary cell
Example 5
Positive electrode active material (Li (Ni 0.8Co0.1Mn0.1)O2), carbon black as a conductive agent, and polyvinylidene fluoride as a binder were added to N-methyl-2-pyrrolidone (NMP) as a solvent in a weight ratio of 98:1:1 to prepare a positive electrode slurry (solid matter 40 wt%). 20 μm thick positive electrode current collector (Al film) was coated with the positive electrode slurry, dried, and rolled to prepare a positive electrode.
Negative electrode active material (artificial graphite: natural graphite: sio=85:10:5, weight ratio), carbon black as a conductive agent, SBR as a binder, and CMC as a thickener were added to NMP at a weight ratio of 95.6:1:2.3:1.1 to prepare a negative electrode slurry (solid: 90 wt%). A copper (Cu) thin film (as a negative electrode current collector) having a thickness of 10 μm was coated with a negative electrode slurry, dried, and rolled to prepare a negative electrode.
After preparing an electrode assembly by stacking the positive electrode, the separator formed of the porous polyethylene film, and the negative electrode prepared above in this order, the electrode assembly was put into a pouch-type battery case, and the nonaqueous electrolyte solution (B-3) for a lithium secondary battery prepared in example 3 was injected thereto, thereby preparing a pouch-type lithium secondary battery.
Example 6
A pouch-type lithium secondary battery was fabricated in the same manner as in example 5, except that the nonaqueous electrolyte solution (B-4) for a lithium secondary battery of example 4 was used instead of the nonaqueous electrolyte solution (B-3) for a lithium secondary battery of example 3.
Comparative example 3
A pouch-type lithium secondary battery was fabricated in the same manner as in example 5, except that the electrolyte solution (a-2) of comparative example 2 was used instead of the nonaqueous electrolyte solution (B-3) for a lithium secondary battery of example 3.
Experimental example
Experimental example 1 evaluation of metal (Co) ion electrodeposition
The nonaqueous electrolyte solutions for lithium secondary batteries of examples 1-1 and 2-1 were prepared by adding 0.1g of cobalt (II) tetrafluoroborate hexahydrate (Co (BF 4)2·6H2 O) (metallic foreign matter, as an optional component) to 99.9g of the nonaqueous electrolyte solutions for lithium secondary batteries (B-1 and B-2) prepared in examples 1 and 2, respectively, to perform metal ion electrodeposition evaluation (see table 1 below).
Further, a nonaqueous electrolyte solution for lithium secondary batteries of comparative example 1-1 was prepared by adding 0.1g of cobalt (II) tetrafluoroborate hexahydrate (Co (BF 4)2·6H2 O) (metallic foreign matter, as an optional component) to 99.9g of the electrolyte solution (a-1) prepared in comparative example 1, to perform metal ion electrodeposition evaluation (see table 1 below).
TABLE 1
Then, electrochemical stability of the electrolyte solution (a-1) free of metal foreign matters prepared in comparative example 1 and the nonaqueous electrolyte solutions for lithium secondary batteries of examples 1-1 and 2-1 and comparative example 1-1 (containing metal foreign matters for metal ion electrodeposition evaluation) was measured using a Linear Sweep Voltammetry (LSV) to evaluate the effect of removing transition metal (Co) ions.
In this case, the working electrode was a platinum (Pt) disk (Φ1.6mm) electrode, the reference electrode was metallic lithium, and a Pt wire electrode was used as an auxiliary electrode, and measurements were made at a scan rate of 10mV/s in the Open Circuit Voltage (OCV) range of about 0.2V. The results of measurement in a glove box (moisture and oxygen concentration of 10ppm or less at 23 ℃) in an argon (Ar) atmosphere are shown in FIG. 1.
Referring to fig. 1, regarding the non-aqueous electrolyte solution for a lithium secondary battery of comparative example 1 without metal foreign matter used as a reference, it can be understood that the current variation between 0.5V and 2.5V is not large.
Regarding the nonaqueous electrolyte solution for lithium secondary batteries of comparative example 1-1 (containing only metallic foreign matters, no additive), it was confirmed that the current rapidly increased between 0.5V and 2.5V due to not only the increase in concentration of free metal (Co) ions in the electrolyte solution but also due to electrodeposition of excessive metal ions on the surface of the Pt disk electrode, which also occurred side reactions.
In contrast, regarding the nonaqueous electrolyte solutions for lithium secondary batteries of examples 1-1 and 2-1 of the present invention (containing the additive and the metallic foreign matter), even if the metallic foreign matter is contained, the rapid increase in current is suppressed, and in particular, regarding the nonaqueous electrolyte solution for lithium secondary batteries of example 2-1 (in which the amount of the additive is large), since the side reaction due to the metallic foreign matter is suppressed more effectively, it can be understood that the current flowing is lower than that of the nonaqueous electrolyte solution for lithium secondary batteries of example 1-1.
The reason for this is due to the fact that: since the amount of the additive in the nonaqueous electrolyte solution for lithium secondary batteries of example 2 is larger than that of the nonaqueous electrolyte solution for lithium secondary batteries of example 1, a complex with metal ions is better formed, thereby reducing the concentration of free Co ions in the electrolyte solution.
Experimental example 2 decomposition initiation Voltage measurement
The decomposition initiation voltages of the nonaqueous electrolyte solution (B-3) for lithium secondary battery prepared in example 3 and the electrolyte solution (A-2) prepared in comparative example 2 were measured using Linear Sweep Voltammetry (LSV).
In this case, the working electrode was a platinum (Pt) disk (Φ1.6mm) electrode, the reference electrode was metallic lithium, and a Pt wire electrode was used as an auxiliary electrode, and measurements were made at a scan rate of 20mV/s in the Open Circuit Voltage (OCV) range of about 6V. The results of measurement in a glove box (moisture and oxygen concentration of 10ppm or less at 23 ℃) in an argon (Ar) atmosphere are shown in FIG. 2.
Referring to fig. 2, regarding the nonaqueous electrolyte solution (B-3) for a lithium secondary battery of example 3, it can be understood that the oxidation current starts at a lower potential than the electrolyte solution (a-2) of comparative example 2.
From these results, since the additive contained in the nonaqueous electrolyte for a lithium secondary battery of the present invention is oxidatively decomposed before the organic solvent during overcharge of the lithium secondary battery to form a film on the surface of the positive electrode, and the film can suppress the decomposition of the organic solvent to suppress the generation of gas due to the decomposition of the organic solvent, it can be predicted that the stability of the lithium secondary battery during overcharge can be ensured.
Experimental example 3 evaluation of SEI formation (1)
After each of the secondary batteries prepared in example 5 and comparative example 3 was initially charged (formed) for 3 hours with a constant current of 0.1C magnification using a PNE-0506 charge-discharge apparatus (manufacturer: PNE state co., ltd.,5v,6 a), a differential capacitance curve obtained by first-order differentiating the capacity-voltage curve thus obtained was shown in fig. 3.
Referring to fig. 3, regarding the lithium secondary battery of example 5, which contained the non-aqueous electrolyte solution of the present invention containing the additive, a decomposition peak (in which the electrolyte solution decomposed at about 1.6V) was confirmed as compared with the secondary battery of comparative example 3, which contained the non-aqueous electrolyte solution containing no additive. From this behavior, it can be indirectly confirmed that the additive contained in the nonaqueous electrolyte solution of the present invention additionally forms another type of SEI on the surface of the negative electrode while decomposing earlier than other components.
Experimental example 4 initial Capacity evaluation test
Each of the secondary batteries prepared in examples 5 and 6 and comparative example 3 was charged to 4.2V at 0.3C rate under constant current-constant voltage (CC-CV) condition at room temperature (23 ℃) and discharged to 2.5V at 0.3C rate under CC condition, and each of the secondary batteries was charged to 1/4.2V at 1C/20 (mA) current reaching 1C under constant current-constant voltage (CC/CV) condition at room temperature (23 ℃) and then discharged to 2.5V at 1C current again to measure initial capacity. The results are shown in table 2 below.
TABLE 2
| 0.33C Capacity (mAh) | |
| Example 5 | 102.5 |
| Example 6 | 98.2 |
| Comparative example 3 | 93.0 |
As shown in table 2, it can be understood that the initial capacity of the secondary battery of comparative example 3 was reduced as compared with the initial capacities of the secondary batteries of examples 5 and 6.
Experimental example 5 evaluation of film formation (2)
After the initial capacity evaluation in experimental example 4 was completed, electrochemical Impedance Spectra (EIS) of each secondary battery of example 5 and comparative example 3 were measured using a potentiostat.
Specifically, after the secondary batteries of example 5 and each of the secondary batteries of comparative example 3 were charged to a charged State (SOC) of 50% at a current of 54mA, a small voltage (14 mv) was applied in a frequency range of 50mHz to 200kHz to measure the generated current response, the results of which are shown in fig. 4.
Referring to fig. 4, regarding the secondary battery of example 5, since a film was formed, it was confirmed that the impedance was increased as compared with that of the secondary battery of comparative example 3. That is, from these results, it was confirmed that a firm film was formed by the additives contained in the nonaqueous electrolyte solution of the present invention.
Experimental example 6 evaluation of high temperature (45 ℃ C.) cycle characteristics
The secondary batteries prepared in example 5 and each of the secondary batteries prepared in comparative example 3 were charged to 4.2V at a constant current/constant voltage (CC-CV) condition at 45C rate until the current reached 1/20 (mA) of 1C, and then discharged to 2.5V at a current of 1C. The charge and discharge were set to one cycle, and 200 cycles were repeated. Next, the discharge capacity retention rate was calculated using the following equation 1, the result of which is shown in fig. 5.
[ Equation 1]
Discharge capacity retention (%) = (discharge capacity after nth charge and discharge/discharge capacity after 1 st charge and discharge) ×100
Referring to fig. 5, regarding the secondary battery of example 5 including the additive of the present invention, it can be understood that the 1C discharge capacity retention rate after the 200 th charge-discharge cycle is greater than that of the secondary battery of comparative example 3. From this, it was confirmed that when coumarin-3-carbonitrile was used as an additive in a nonaqueous electrolyte solution, the high-rate discharge capacity retention rate at high temperature could be improved.
Claims (6)
1.A nonaqueous electrolyte solution for a lithium secondary battery, the nonaqueous electrolyte solution comprising a lithium salt, an organic solvent, and a compound represented by formula 1 as an additive:
[ 1]
Wherein, in the formula 1,
R 1 is a-CN group, R 2 is hydrogen or an alkyl group having 1 to 3 carbon atoms, and R 3 to R 6 are each independently hydrogen, an alkyl group having 1 to 3 carbon atoms or a-CN group, and
Wherein the compound represented by formula 1 is contained in an amount of 0.05 wt% or more and less than 1.2 wt% based on the total weight of the nonaqueous electrolyte solution.
2. The nonaqueous electrolyte solution for lithium secondary batteries according to claim 1, wherein in formula 1, R 1 is a-CN group, R 2 is hydrogen, R 3 and R 6 are each independently hydrogen or a-CN group, and R 4 and R 5 are each independently hydrogen, an alkyl group having 1 to 3 carbon atoms, or a-CN group.
3. The nonaqueous electrolyte solution for lithium secondary batteries according to claim 1, wherein the compound represented by formula 1 comprises a compound represented by formula 1 a:
[ 1a ]
4. The nonaqueous electrolyte solution for lithium secondary batteries according to claim 1, wherein the compound represented by formula 1 is contained in an amount of 0.1 to 1% by weight based on the total weight of the nonaqueous electrolyte solution.
5. A lithium secondary battery includes a negative electrode, a positive electrode, a separator disposed between the negative electrode and the positive electrode, and a nonaqueous electrolyte solution,
Wherein the nonaqueous electrolyte solution comprises the nonaqueous electrolyte solution for a lithium secondary battery according to claim 1.
6. The lithium secondary battery according to claim 5, wherein the positive electrode comprises a positive electrode active material comprising lithium and at least one metal selected from the group consisting of nickel (Ni), cobalt (Co), manganese (Mn), iron (Fe), and aluminum (Al).
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| KR1020200151165A KR102633527B1 (en) | 2019-11-18 | 2020-11-12 | Non-aqueous electrolyte for lithium secondary battery and lithium secondary battery comprising the same |
| PCT/KR2020/015946 WO2021101174A1 (en) | 2019-11-18 | 2020-11-13 | Non-aqueous electrolyte solution for lithium secondary battery and lithium secondary battery comprising same |
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| EP4329038A1 (en) * | 2021-08-06 | 2024-02-28 | LG Energy Solution, Ltd. | Non-aqueous electrolyte comprising additive for non-aqueous electrolyte, and lithium secondary battery comprising same |
| CA3217209A1 (en) * | 2021-08-06 | 2023-02-09 | Lg Energy Solution, Ltd. | Non-aqueous electrolyte including additive for non-aqueous electrolyte and lithium secondary battery including the same |
| JP2024520516A (en) * | 2021-10-05 | 2024-05-24 | エルジー エナジー ソリューション リミテッド | Nonaqueous electrolyte for lithium secondary battery and lithium secondary battery containing same |
| CA3219953A1 (en) * | 2021-11-12 | 2023-05-19 | Lg Energy Solution, Ltd. | Non-aqueous electrolyte including additive for non-aqueous electrolyte, and lithium secondary battery including the non-aqueous electrolyte |
| EP4336617A1 (en) * | 2021-12-01 | 2024-03-13 | LG Energy Solution, Ltd. | Non-aqueous electrolyte for lithium secondary battery, and lithium secondary battery comprising same |
| US20230253624A1 (en) * | 2022-02-08 | 2023-08-10 | Lg Energy Solution, Ltd. | Non-Aqueous Electrolyte and Lithium Secondary Battery Including the Same |
| CA3237191A1 (en) * | 2022-05-13 | 2023-11-16 | Lg Energy Solution, Ltd. | Non-aqueous electrolyte and lithium secondary battery including the same |
| KR102650157B1 (en) * | 2022-05-13 | 2024-03-22 | 주식회사 엘지에너지솔루션 | Non-aqueous electrolyte and lithium secondary battery comprising the same |
| WO2024014788A1 (en) * | 2022-07-12 | 2024-01-18 | 주식회사 엘지에너지솔루션 | Non-aqueous electrolyte for lithium secondary battery and lithium secondary battery comprising same |
| KR20240022933A (en) * | 2022-08-12 | 2024-02-20 | 주식회사 엘지에너지솔루션 | Non-aqueous electrolyte and lithium secondary battery comprising the same |
| WO2024039232A1 (en) * | 2022-08-18 | 2024-02-22 | 주식회사 엘지에너지솔루션 | Lithium secondary battery |
| KR20240045912A (en) * | 2022-09-30 | 2024-04-08 | 주식회사 엘지에너지솔루션 | Non-aqueous electrolyte and lithium secondary battery comprising the same |
| KR20240045913A (en) * | 2022-09-30 | 2024-04-08 | 주식회사 엘지에너지솔루션 | Non-aqueous electrolyte and lithium secondary battery comprising the same |
| WO2024122996A1 (en) * | 2022-12-09 | 2024-06-13 | 주식회사 엘지에너지솔루션 | Lithium secondary battery |
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