WO2022255669A1 - 양극 첨가제 및 이를 함유하는 리튬 이차전지용 양극 - Google Patents
양극 첨가제 및 이를 함유하는 리튬 이차전지용 양극 Download PDFInfo
- Publication number
- WO2022255669A1 WO2022255669A1 PCT/KR2022/006465 KR2022006465W WO2022255669A1 WO 2022255669 A1 WO2022255669 A1 WO 2022255669A1 KR 2022006465 W KR2022006465 W KR 2022006465W WO 2022255669 A1 WO2022255669 A1 WO 2022255669A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- mixture layer
- positive electrode
- secondary battery
- lithium secondary
- binder
- Prior art date
Links
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 72
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 67
- 239000000654 additive Substances 0.000 title claims abstract description 56
- 230000000996 additive effect Effects 0.000 title claims abstract description 53
- 239000000203 mixture Substances 0.000 claims abstract description 197
- 239000011230 binding agent Substances 0.000 claims abstract description 92
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 32
- 238000004519 manufacturing process Methods 0.000 claims abstract description 18
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 33
- 239000011347 resin Substances 0.000 claims description 32
- 229920005989 resin Polymers 0.000 claims description 32
- 239000004020 conductor Substances 0.000 claims description 29
- 239000002131 composite material Substances 0.000 claims description 23
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims description 21
- 229910052731 fluorine Inorganic materials 0.000 claims description 21
- 239000011737 fluorine Substances 0.000 claims description 21
- 239000006182 cathode active material Substances 0.000 claims description 17
- 229920001971 elastomer Polymers 0.000 claims description 15
- 239000007774 positive electrode material Substances 0.000 claims description 15
- 239000005060 rubber Substances 0.000 claims description 15
- 230000003068 static effect Effects 0.000 claims description 15
- 229910052719 titanium Inorganic materials 0.000 claims description 15
- 229910052782 aluminium Inorganic materials 0.000 claims description 14
- 239000000126 substance Substances 0.000 claims description 14
- 229910052802 copper Inorganic materials 0.000 claims description 13
- 229910052804 chromium Inorganic materials 0.000 claims description 12
- 229910052742 iron Inorganic materials 0.000 claims description 11
- 229910052749 magnesium Inorganic materials 0.000 claims description 11
- 239000000178 monomer Substances 0.000 claims description 11
- 229910052684 Cerium Inorganic materials 0.000 claims description 10
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 10
- 229910052772 Samarium Inorganic materials 0.000 claims description 10
- 229910052789 astatine Inorganic materials 0.000 claims description 10
- 229910052796 boron Inorganic materials 0.000 claims description 10
- 229910052791 calcium Inorganic materials 0.000 claims description 10
- 229910052738 indium Inorganic materials 0.000 claims description 10
- 229910052746 lanthanum Inorganic materials 0.000 claims description 10
- 229910052750 molybdenum Inorganic materials 0.000 claims description 10
- 229910052758 niobium Inorganic materials 0.000 claims description 10
- 229910052712 strontium Inorganic materials 0.000 claims description 10
- 229910052721 tungsten Inorganic materials 0.000 claims description 10
- 229910052720 vanadium Inorganic materials 0.000 claims description 10
- 229910052725 zinc Inorganic materials 0.000 claims description 10
- 229910052726 zirconium Inorganic materials 0.000 claims description 10
- 229910021382 natural graphite Inorganic materials 0.000 claims description 9
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 8
- 239000002041 carbon nanotube Substances 0.000 claims description 8
- 229910021389 graphene Inorganic materials 0.000 claims description 8
- 229920003048 styrene butadiene rubber Polymers 0.000 claims description 8
- MIZLGWKEZAPEFJ-UHFFFAOYSA-N 1,1,2-trifluoroethene Chemical group FC=C(F)F MIZLGWKEZAPEFJ-UHFFFAOYSA-N 0.000 claims description 7
- 229910021383 artificial graphite Inorganic materials 0.000 claims description 7
- 229920000642 polymer Polymers 0.000 claims description 7
- BQCIDUSAKPWEOX-UHFFFAOYSA-N 1,1-Difluoroethene Chemical compound FC(F)=C BQCIDUSAKPWEOX-UHFFFAOYSA-N 0.000 claims description 6
- QMIWYOZFFSLIAK-UHFFFAOYSA-N 3,3,3-trifluoro-2-(trifluoromethyl)prop-1-ene Chemical group FC(F)(F)C(=C)C(F)(F)F QMIWYOZFFSLIAK-UHFFFAOYSA-N 0.000 claims description 6
- GVEUEBXMTMZVSD-UHFFFAOYSA-N 3,3,4,4,5,5,6,6,6-nonafluorohex-1-ene Chemical group FC(F)(F)C(F)(F)C(F)(F)C(F)(F)C=C GVEUEBXMTMZVSD-UHFFFAOYSA-N 0.000 claims description 6
- UUAGAQFQZIEFAH-UHFFFAOYSA-N chlorotrifluoroethylene Chemical group FC(F)=C(F)Cl UUAGAQFQZIEFAH-UHFFFAOYSA-N 0.000 claims description 6
- HCDGVLDPFQMKDK-UHFFFAOYSA-N hexafluoropropylene Chemical compound FC(F)=C(F)C(F)(F)F HCDGVLDPFQMKDK-UHFFFAOYSA-N 0.000 claims description 6
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 claims description 6
- XUCNUKMRBVNAPB-UHFFFAOYSA-N fluoroethene Chemical compound FC=C XUCNUKMRBVNAPB-UHFFFAOYSA-N 0.000 claims description 5
- 239000002905 metal composite material Substances 0.000 claims description 5
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 4
- 239000006230 acetylene black Substances 0.000 claims description 4
- 239000004917 carbon fiber Substances 0.000 claims description 4
- 238000007580 dry-mixing Methods 0.000 claims description 4
- 239000003273 ketjen black Substances 0.000 claims description 4
- NDMMKOCNFSTXRU-UHFFFAOYSA-N 1,1,2,3,3-pentafluoroprop-1-ene Chemical compound FC(F)C(F)=C(F)F NDMMKOCNFSTXRU-UHFFFAOYSA-N 0.000 claims description 3
- FDMFUZHCIRHGRG-UHFFFAOYSA-N 3,3,3-trifluoroprop-1-ene Chemical compound FC(F)(F)C=C FDMFUZHCIRHGRG-UHFFFAOYSA-N 0.000 claims description 3
- 229920000459 Nitrile rubber Polymers 0.000 claims description 3
- 239000005062 Polybutadiene Substances 0.000 claims description 3
- KLIYQWXIWMRMGR-UHFFFAOYSA-N buta-1,3-diene;methyl 2-methylprop-2-enoate Chemical compound C=CC=C.COC(=O)C(C)=C KLIYQWXIWMRMGR-UHFFFAOYSA-N 0.000 claims description 3
- MTAZNLWOLGHBHU-UHFFFAOYSA-N butadiene-styrene rubber Chemical class C=CC=C.C=CC1=CC=CC=C1 MTAZNLWOLGHBHU-UHFFFAOYSA-N 0.000 claims description 3
- RKTYLMNFRDHKIL-UHFFFAOYSA-N copper;5,10,15,20-tetraphenylporphyrin-22,24-diide Chemical group [Cu+2].C1=CC(C(=C2C=CC([N-]2)=C(C=2C=CC=CC=2)C=2C=CC(N=2)=C(C=2C=CC=CC=2)C2=CC=C3[N-]2)C=2C=CC=CC=2)=NC1=C3C1=CC=CC=C1 RKTYLMNFRDHKIL-UHFFFAOYSA-N 0.000 claims description 3
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 3
- 229920001084 poly(chloroprene) Polymers 0.000 claims description 3
- 229920002857 polybutadiene Polymers 0.000 claims description 3
- 239000000853 adhesive Substances 0.000 abstract description 4
- 230000001070 adhesive effect Effects 0.000 abstract description 4
- 230000002209 hydrophobic effect Effects 0.000 abstract description 4
- 239000002245 particle Substances 0.000 description 25
- 238000000034 method Methods 0.000 description 18
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 18
- -1 etc. may be used Chemical compound 0.000 description 17
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 15
- 230000002427 irreversible effect Effects 0.000 description 15
- 239000010936 titanium Substances 0.000 description 13
- 239000003575 carbonaceous material Substances 0.000 description 11
- 230000000052 comparative effect Effects 0.000 description 10
- 239000010949 copper Substances 0.000 description 10
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 10
- 239000002210 silicon-based material Substances 0.000 description 10
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 9
- 239000011651 chromium Substances 0.000 description 9
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 9
- 239000011777 magnesium Substances 0.000 description 9
- 239000011701 zinc Substances 0.000 description 9
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 8
- 239000011267 electrode slurry Substances 0.000 description 8
- 239000011572 manganese Substances 0.000 description 8
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 7
- 229910052759 nickel Inorganic materials 0.000 description 7
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 description 6
- 239000002033 PVDF binder Substances 0.000 description 6
- 229910052799 carbon Inorganic materials 0.000 description 6
- 239000013078 crystal Substances 0.000 description 6
- 239000008151 electrolyte solution Substances 0.000 description 6
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 6
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 6
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 6
- 239000007784 solid electrolyte Substances 0.000 description 6
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 5
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 5
- 230000008901 benefit Effects 0.000 description 5
- 238000001035 drying Methods 0.000 description 5
- 239000010408 film Substances 0.000 description 5
- 239000010703 silicon Substances 0.000 description 5
- 229910052710 silicon Inorganic materials 0.000 description 5
- 239000002904 solvent Substances 0.000 description 5
- 229910011328 LiNi0.6Co0.2Mn0.2O2 Inorganic materials 0.000 description 4
- 239000004698 Polyethylene Substances 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 229910017052 cobalt Inorganic materials 0.000 description 4
- 239000010941 cobalt Substances 0.000 description 4
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 4
- 239000003792 electrolyte Substances 0.000 description 4
- 229910002804 graphite Inorganic materials 0.000 description 4
- 239000010439 graphite Substances 0.000 description 4
- 239000007773 negative electrode material Substances 0.000 description 4
- 239000004745 nonwoven fabric Substances 0.000 description 4
- 229920000573 polyethylene Polymers 0.000 description 4
- 239000007787 solid Substances 0.000 description 4
- 229910001220 stainless steel Inorganic materials 0.000 description 4
- 239000010935 stainless steel Substances 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 3
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- 229910013716 LiNi Inorganic materials 0.000 description 3
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 3
- 239000006183 anode active material Substances 0.000 description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 239000001569 carbon dioxide Substances 0.000 description 3
- 238000007599 discharging Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000011156 evaluation Methods 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- 229910003002 lithium salt Inorganic materials 0.000 description 3
- 159000000002 lithium salts Chemical class 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 238000007086 side reaction Methods 0.000 description 3
- 229910052814 silicon oxide Inorganic materials 0.000 description 3
- AHVCRWLQBFGUKH-UHFFFAOYSA-N 1,1,1,4-tetrafluorobut-2-ene Chemical compound FCC=CC(F)(F)F AHVCRWLQBFGUKH-UHFFFAOYSA-N 0.000 description 2
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 description 2
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- ZHNUHDYFZUAESO-UHFFFAOYSA-N Formamide Chemical compound NC=O ZHNUHDYFZUAESO-UHFFFAOYSA-N 0.000 description 2
- 229910015872 LiNi0.8Co0.1Mn0.1O2 Inorganic materials 0.000 description 2
- 229910013870 LiPF 6 Inorganic materials 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- JUJWROOIHBZHMG-UHFFFAOYSA-N Pyridine Chemical compound C1=CC=NC=C1 JUJWROOIHBZHMG-UHFFFAOYSA-N 0.000 description 2
- KAESVJOAVNADME-UHFFFAOYSA-N Pyrrole Chemical class C=1C=CNC=1 KAESVJOAVNADME-UHFFFAOYSA-N 0.000 description 2
- 229910004298 SiO 2 Inorganic materials 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- 239000006229 carbon black Substances 0.000 description 2
- 239000006257 cathode slurry Substances 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 2
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 description 2
- LYCAIKOWRPUZTN-UHFFFAOYSA-N ethylene glycol Natural products OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 2
- 239000006260 foam Substances 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 229910003480 inorganic solid Inorganic materials 0.000 description 2
- AMXOYNBUYSYVKV-UHFFFAOYSA-M lithium bromide Chemical compound [Li+].[Br-] AMXOYNBUYSYVKV-UHFFFAOYSA-M 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- 229910001416 lithium ion Inorganic materials 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical compound COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000011356 non-aqueous organic solvent Substances 0.000 description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 2
- 239000000377 silicon dioxide Substances 0.000 description 2
- 235000012239 silicon dioxide Nutrition 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- VZGDMQKNWNREIO-UHFFFAOYSA-N tetrachloromethane Chemical compound ClC(Cl)(Cl)Cl VZGDMQKNWNREIO-UHFFFAOYSA-N 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- PYOKUURKVVELLB-UHFFFAOYSA-N trimethyl orthoformate Chemical compound COC(OC)OC PYOKUURKVVELLB-UHFFFAOYSA-N 0.000 description 2
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 description 1
- CYSGHNMQYZDMIA-UHFFFAOYSA-N 1,3-Dimethyl-2-imidazolidinon Chemical compound CN1CCN(C)C1=O CYSGHNMQYZDMIA-UHFFFAOYSA-N 0.000 description 1
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 1
- XNWFRZJHXBZDAG-UHFFFAOYSA-N 2-METHOXYETHANOL Chemical class COCCO XNWFRZJHXBZDAG-UHFFFAOYSA-N 0.000 description 1
- JWUJQDFVADABEY-UHFFFAOYSA-N 2-methyltetrahydrofuran Chemical compound CC1CCCO1 JWUJQDFVADABEY-UHFFFAOYSA-N 0.000 description 1
- PPDFQRAASCRJAH-UHFFFAOYSA-N 2-methylthiolane 1,1-dioxide Chemical compound CC1CCCS1(=O)=O PPDFQRAASCRJAH-UHFFFAOYSA-N 0.000 description 1
- XMWRBQBLMFGWIX-UHFFFAOYSA-N C60 fullerene Chemical class C12=C3C(C4=C56)=C7C8=C5C5=C9C%10=C6C6=C4C1=C1C4=C6C6=C%10C%10=C9C9=C%11C5=C8C5=C8C7=C3C3=C7C2=C1C1=C2C4=C6C4=C%10C6=C9C9=C%11C5=C5C8=C3C3=C7C1=C1C2=C4C6=C2C9=C5C3=C12 XMWRBQBLMFGWIX-UHFFFAOYSA-N 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical class [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 1
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical compound NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 description 1
- 229910012722 Li3N-LiI-LiOH Inorganic materials 0.000 description 1
- 229910012716 Li3N-LiI—LiOH Inorganic materials 0.000 description 1
- 229910012734 Li3N—LiI—LiOH Inorganic materials 0.000 description 1
- 229910013043 Li3PO4-Li2S-SiS2 Inorganic materials 0.000 description 1
- 229910013035 Li3PO4-Li2S—SiS2 Inorganic materials 0.000 description 1
- 229910012810 Li3PO4—Li2S-SiS2 Inorganic materials 0.000 description 1
- 229910012797 Li3PO4—Li2S—SiS2 Inorganic materials 0.000 description 1
- 229910012047 Li4SiO4-LiI-LiOH Inorganic materials 0.000 description 1
- 229910012075 Li4SiO4-LiI—LiOH Inorganic materials 0.000 description 1
- 229910012057 Li4SiO4—LiI—LiOH Inorganic materials 0.000 description 1
- 229910010238 LiAlCl 4 Inorganic materials 0.000 description 1
- 229910015015 LiAsF 6 Inorganic materials 0.000 description 1
- 229910013063 LiBF 4 Inorganic materials 0.000 description 1
- 229910013684 LiClO 4 Inorganic materials 0.000 description 1
- 229910012513 LiSbF 6 Inorganic materials 0.000 description 1
- 229910012573 LiSiO Inorganic materials 0.000 description 1
- 229910012346 LiSiO4-LiI-LiOH Inorganic materials 0.000 description 1
- 229910012345 LiSiO4-LiI—LiOH Inorganic materials 0.000 description 1
- 229910012348 LiSiO4—LiI—LiOH Inorganic materials 0.000 description 1
- 229910001228 Li[Ni1/3Co1/3Mn1/3]O2 (NCM 111) Inorganic materials 0.000 description 1
- KDXKERNSBIXSRK-UHFFFAOYSA-N Lysine Natural products NCCCCC(N)C(O)=O KDXKERNSBIXSRK-UHFFFAOYSA-N 0.000 description 1
- 239000004472 Lysine Substances 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- ZHGDJTMNXSOQDT-UHFFFAOYSA-N NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O Chemical compound NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O ZHGDJTMNXSOQDT-UHFFFAOYSA-N 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 1
- 229910004283 SiO 4 Inorganic materials 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical class C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 1
- GSEJCLTVZPLZKY-UHFFFAOYSA-N Triethanolamine Chemical compound OCCN(CCO)CCO GSEJCLTVZPLZKY-UHFFFAOYSA-N 0.000 description 1
- BEKPOUATRPPTLV-UHFFFAOYSA-N [Li].BCl Chemical compound [Li].BCl BEKPOUATRPPTLV-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
- 239000002253 acid Substances 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 238000013019 agitation Methods 0.000 description 1
- 150000007933 aliphatic carboxylic acids Chemical class 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical class Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 description 1
- 150000003863 ammonium salts Chemical class 0.000 description 1
- 239000006256 anode slurry Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 229910002090 carbon oxide Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 229910000428 cobalt oxide Inorganic materials 0.000 description 1
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 1
- 150000004292 cyclic ethers Chemical class 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 238000009831 deintercalation Methods 0.000 description 1
- 229940113088 dimethylacetamide Drugs 0.000 description 1
- 150000004862 dioxolanes Chemical class 0.000 description 1
- 229910001882 dioxygen Inorganic materials 0.000 description 1
- 238000010494 dissociation reaction Methods 0.000 description 1
- 230000005593 dissociations Effects 0.000 description 1
- 238000010828 elution Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 229910003472 fullerene Inorganic materials 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- 150000004820 halides Chemical class 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
- 150000002461 imidazolidines Chemical class 0.000 description 1
- 150000003949 imides Chemical class 0.000 description 1
- 239000010954 inorganic particle Substances 0.000 description 1
- 238000009830 intercalation Methods 0.000 description 1
- 230000002687 intercalation Effects 0.000 description 1
- 230000010220 ion permeability Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 235000015110 jellies Nutrition 0.000 description 1
- 239000008274 jelly Substances 0.000 description 1
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 description 1
- 229910001947 lithium oxide Inorganic materials 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 239000002071 nanotube Substances 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 150000005181 nitrobenzenes Chemical class 0.000 description 1
- LYGJENNIWJXYER-UHFFFAOYSA-N nitromethane Chemical compound C[N+]([O-])=O LYGJENNIWJXYER-UHFFFAOYSA-N 0.000 description 1
- 229910021470 non-graphitizable carbon Inorganic materials 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- 239000011146 organic particle Substances 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-N phosphoric acid Substances OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 1
- 150000003014 phosphoric acid esters Chemical class 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
- 229920000307 polymer substrate Polymers 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 229920001451 polypropylene glycol Polymers 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 239000008213 purified water Substances 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- 239000001008 quinone-imine dye Substances 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- VSZWPYCFIRKVQL-UHFFFAOYSA-N selanylidenegallium;selenium Chemical compound [Se].[Se]=[Ga].[Se]=[Ga] VSZWPYCFIRKVQL-UHFFFAOYSA-N 0.000 description 1
- 230000001568 sexual effect Effects 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 238000004381 surface treatment Methods 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 1
- BDZBKCUKTQZUTL-UHFFFAOYSA-N triethyl phosphite Chemical compound CCOP(OCC)OCC BDZBKCUKTQZUTL-UHFFFAOYSA-N 0.000 description 1
Classifications
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- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
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- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
- H01M4/622—Binders being polymers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
- H01M4/622—Binders being polymers
- H01M4/623—Binders being polymers fluorinated polymers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
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- 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
Definitions
- the present invention relates to a cathode additive for a lithium secondary battery and a cathode for a lithium secondary battery containing the same.
- lithium secondary batteries having high energy density and operating potential, long cycle life, and low self-discharge rate have been commercialized and widely used.
- lithium secondary batteries are used as a power source for medium-large devices such as electric vehicles, high capacity, high energy density, and low cost of lithium secondary batteries are further demanded, and higher irreversible capacity is required for irreversible additives used in electrodes. something is being demanded However, it is true that there is a limit to the development of a positive electrode additive having such a high irreversible capacity.
- irreversible additives such as Li 6 CoO 4 are generally prepared by reacting cobalt oxide or the like with an excess of lithium oxide.
- the irreversible additive prepared in this way is structurally unstable and may decompose and lose irreversible activity when a cathode is manufactured under conditions of high temperature and/or high humidity, and as charging proceeds, oxygen gas (O 2 ) and carbon dioxide (CO 2 ) ) and the like are generated, and the generated gas causes volume expansion of the electrode assembly, thereby degrading the stability of the battery, and carbon oxides of carbon dioxide (CO 2 ) induce a side reaction that decomposes the battery. can act as a major factor that causes the performance degradation of
- a binder is used in the positive electrode mixture layer in order to secure adhesion between the positive electrode active material and the irreversible additive and between the positive electrode active material and the current collector.
- the adhesive strength of the binder may be reduced depending on the type of cathode active material, the surface condition of the current collector, etc., and when the content of the binder is increased to prevent this, there is a limit to the decrease in the capacity and electrical conductivity of the electrode due to the excess binder. have.
- an object of the present invention is to contain an irreversible additive in a positive electrode mixture layer provided in a positive electrode, to minimize damage to the irreversible additive, and to improve the adhesion between the positive electrode mixture layer and the positive electrode current collector, thereby improving the electrical performance and lifespan of the battery. It is to provide a positive electrode for a lithium secondary battery that can be improved and a lithium secondary battery having the same.
- the present invention in one embodiment, the present invention
- It has a structure in which a cathode current collector, a first mixture layer, and a second mixture layer are sequentially stacked;
- the first mixture layer includes a first binder made of a rubber-based resin,
- the second mixture layer provides a positive electrode for a lithium secondary battery including a second binder composed of a fluorine-based resin derived from a fluorine (F)-containing monomer.
- the difference between the static water contact angle of the first mixture layer and the static water contact angle of the second mixture layer may be 5° or more, specifically, 10° to 30°.
- the rubber-based resin may include at least one selected from the group consisting of styrene-butadiene rubber, nitrile-butadiene rubber, methyl methacrylate-butadiene rubber, chloroprene rubber, carboxy-modified styrene-butadiene rubber, and modified polyorganosiloxane polymers.
- styrene-butadiene rubber nitrile-butadiene rubber, methyl methacrylate-butadiene rubber, chloroprene rubber, carboxy-modified styrene-butadiene rubber, and modified polyorganosiloxane polymers.
- the fluorine-based resin is vinylidene fluoride (VDF or VF2), tetrafluoroethylene (TFE), trifluoroethylene (TrFE), chlorotrifluoroethylene (CTFE), hexafluoropropene (HFP), Vinyl fluoride (VF), hexafluoroisobutylene (HFIB), perfluorobutylethylene (PFBE), pentafluoropropene, 3,3,3-trifluoro-1-propene and 2-tri and a resin derived from one or more monomers selected from the group consisting of fluoromethyl-3,3,3-trifluoropropene.
- VDF or VF2 vinylidene fluoride
- TFE tetrafluoroethylene
- TrFE trifluoroethylene
- CTFE chlorotrifluoroethylene
- HFP hexafluoropropene
- VF Vinyl fluoride
- HFIB hexafluoroisobutylene
- the amount of the first binder may be 0.5 to 5 parts by weight based on 100 parts by weight of the first mixture layer
- the content of the second binder may be 0.5 to 10 parts by weight based on 100 parts by weight of the second mixture layer.
- the total amount of the first binder and the second binder may be 0.1 to 5 parts by weight based on 100 parts by weight of the total mixture layer.
- At least one of the first mixture layer and the second mixture layer may contain a positive electrode additive represented by Formula 1 below:
- M 1 is W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and At least one element selected from the group consisting of Mo,
- p and q are 5 ⁇ p ⁇ 7 and 0 ⁇ q ⁇ 0.5, respectively.
- the positive electrode additive may be included in an amount of 0.1 to 5 parts by weight based on 100 parts by weight of each positive electrode mixture layer.
- the positive electrode additive may have a tetragonal structure having a space group of P4 2 /nmc.
- the first mixture layer may include a first cathode active material, a first conductive material, a cathode additive, and a first binder
- the second mixture layer may include a second cathode active material, a second conductive material, and a second binder.
- first positive electrode active material and the second positive electrode active material may each include a lithium metal composite oxide represented by Chemical Formula 2:
- M 2 is W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and At least one element selected from the group consisting of Mo,
- x, y, z, w, v and u are 1.0 ⁇ x ⁇ 1.30, 0.1 ⁇ y ⁇ 0.95, 0.01 ⁇ z ⁇ 0.5, 0.01 ⁇ w ⁇ 0.5, 0 ⁇ v ⁇ 0.2, 1.5 ⁇ u ⁇ 4.5, respectively.
- first conductive material and the second conductive material may include at least one selected from the group consisting of natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, carbon nanotube, graphene, and carbon fiber, respectively. have.
- the content of the first conductive material and the second conductive material may be 0.5 to 5 parts by weight based on 100 parts by weight of the positive electrode mixture layer.
- a method for manufacturing a positive electrode for a lithium secondary battery comprising forming a second mixture layer containing a second binder composed of a fluorine-based resin derived from a fluorine (F)-containing monomer on the first mixture layer.
- At least one of the first mixture layer and the second mixture layer may contain a positive electrode additive represented by Formula 1 below:
- M 1 is W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and At least one element selected from the group consisting of Mo,
- p and q are 5 ⁇ p ⁇ 7 and 0 ⁇ q ⁇ 0.5, respectively.
- the forming of the first mixture layer may include preparing a mixture composition by dry mixing a first cathode active material, a cathode additive represented by Chemical Formula 1, a first conductive material, and a first binder composed of a rubber-based resin; and applying the prepared composite material composition on the positive electrode current collector.
- a positive electrode for a lithium secondary battery according to the present invention has a structure in which a positive electrode current collector, a first mixture layer, and a second mixture layer are sequentially stacked, and a binder that is more hydrophobic than the binder contained in the second mixture layer is mixed with the positive electrode collector.
- the first mixture layer adjacent to the first mixture layer the adhesion between the cathode current collector and the mixture layer can be further improved, and thus durability of the cathode can be improved.
- the first mixture layer contains a cathode additive, damage to the cathode additive during cathode manufacturing can be minimized due to the first binder having low affinity for water, thereby further improving the electrical performance and lifespan of the lithium secondary battery.
- the term "comprises” or “has” is intended to designate that there is a feature, number, step, operation, component, part, or combination thereof described in the specification, but one or more other features It should be understood that the presence or addition of numbers, steps, operations, components, parts, or combinations thereof is not precluded.
- a part such as a layer, film, region, plate, etc. when a part such as a layer, film, region, plate, etc. is described as being “on” another part, this includes not only the case where it is “directly on” the other part, but also the case where another part is present in the middle thereof. . Conversely, when a part such as a layer, film, region, plate, or the like is described as being “under” another part, this includes not only being “directly under” the other part, but also the case where there is another part in the middle. In addition, in the present application, being disposed “on” may include the case of being disposed not only on the upper part but also on the lower part.
- main component is 50% by weight or more, 60% by weight or more, 70% by weight or more, 80% by weight or more, 90% by weight or more, 95% by weight or more, or 97.5% by weight or more based on the total weight of the composition or specific component. It may mean more than % by weight, and in some cases, it may mean the case of constituting the entire composition or specific component, that is, 100% by weight.
- Ah is a capacity unit of a lithium secondary battery, and is referred to as an "ampere hour” and means an amount of current per hour. For example, if the battery capacity is “3000 mAh”, it means that it can be discharged for 1 hour with a current of 3000 mA.
- contact angle refers to an angle formed between the liquid surface and the solid wall when the liquid contacts the solid surface.
- the present invention in one embodiment, the present invention
- It has a structure in which a current collector, a first mixture layer, and a second mixture layer are sequentially stacked;
- the first mixture layer includes a first binder made of a rubber-based resin,
- the second mixture layer includes a second binder composed of a fluorine-based resin derived from a fluorine (F)-containing monomer,
- a positive electrode for a lithium secondary battery containing a positive electrode additive represented by Formula 1 in at least one of the first mixture layer and the second mixture layer:
- M 1 is W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and At least one element selected from the group consisting of Mo,
- p and q are 5 ⁇ p ⁇ 7 and 0 ⁇ q ⁇ 0.5, respectively.
- the positive electrode for a lithium secondary battery according to the present invention has a structure including a two-layered mixture layer on a positive electrode current collector, wherein the mixture layer constituting the two-layer structure, specifically, the first mixture layer and the second mixture layer are water It may include heterogeneous binders having different affinity for.
- the first mixture layer contains, as the first binder, a binder made of a rubber-based resin having low affinity for water.
- the first binder may include at least one selected from the group consisting of styrene-butadiene rubber, nitrile-butadiene rubber, methyl methacrylate-butadiene rubber, chloroprene rubber, carboxy-modified styrene-butadiene rubber, and modified polyorganosiloxane polymer.
- the second mixture layer contains, as the second binder, a binder composed of a fluorine-based resin derived from a fluorine (F)-containing monomer having a higher affinity for water.
- a binder composed of a fluorine-based resin derived from a fluorine (F)-containing monomer having a higher affinity for water.
- Such second binders include vinylidene fluoride (VDF or VF2), tetrafluoroethylene (TFE), trifluoroethylene (TrFE), chlorotrifluoroethylene (CTFE), hexafluoropropene (HFP), Vinyl fluoride (VF), hexafluoroisobutylene (HFIB), perfluorobutylethylene (PFBE), pentafluoropropene, 3,3,3-trifluoro-1-propene and 2-tri and a resin derived from one or more monomers selected from the group consisting of fluoromethyl-3,3,3-trifluoropropene
- the second binder may have a crystalline phase and/or an amorphous phase in the positive electrode mixture layer, but specifically, may have both a crystalline phase and an amorphous phase, of which the amorphous phase accounts for 51% or more or 55% or more of the total crystalline phase. can occupy
- the second binder is 51 to 95% of the amorphous phase of the total crystal phase; 51 to 90%; 51 to 85%; 51 to 80%; 51 to 75%; 51 to 70%; 51 to 65%; or 51 to 55%.
- the second binder may have different affinity for water depending on the crystal phase in the mixture layer. Among them, when the crystal form is amorphous, the affinity for water may be high. In the present invention, wettability of the second mixture layer to the electrolyte may be improved by containing the amorphous phase in the total crystal phase of the second binder to exceed 50%.
- a rubber-based resin is contained as a first binder in the first mixture layer adjacent to the positive electrode current collector, and a fluorine-based resin derived from a fluorine (F)-containing monomer is contained in the second mixture layer as a second binder.
- the rubber-based resin as the first binder may have lower affinity for water than the fluorine-based resin as the second binder.
- the deviation between the static water contact angle of the first mixture layer and the static water contact angle of the second mixture layer may be 5° or more, specifically 10° or more; more than 15°; more than 20°; 5° to 30°; 10° to 30°; 15° to 30°; 20° to 30°; 5° to 20°; 5° to 15°; 8° to 15°; 10° to 16°; 14° to 19°; Or it may be 5° to 10°.
- the present invention controls the static water contact angle deviation of the first mixture layer and the second mixture layer within the above range, thereby improving the adhesion between the positive electrode current collector and the first mixture layer; and adhesion between the first mixture layer and the second mixture layer may be improved, and at the same time, wettability of the second mixture layer with respect to the electrolyte solution may be improved.
- the first mixture layer may have a relatively lower affinity for water than the second mixture layer, and may have excellent adhesion to a metal cathode current collector.
- the positive electrode current collector and the mixture layer may be 1.5 times or more strong, and more specifically, 1.8 times or more, 2 times or more, 2.2 times or more, or 2.5 times or more.
- the amount of the first binder may be 0.5 to 5 parts by weight based on 100 parts by weight of the first mixture layer
- the content of the second binder may be 0.5 to 10 parts by weight based on 100 parts by weight of the second mixture layer.
- a total amount of the binder and the second binder may be 0.1 to 5 parts by weight based on 100 parts by weight of the total mixture layer.
- the amount of the first binder is 0.5 to 4 parts by weight based on 100 parts by weight of the first mixture layer; 0.5 to 3 parts by weight; 0.5 to 2 parts by weight; 1 to 3 parts by weight; 2 to 5 parts by weight; or 1.5 to 2.5 parts by weight
- the content of the second binder is 0.5 to 8 parts by weight based on 100 parts by weight of the second mixture layer; 0.5 to 6 parts by weight; 0.5 to 5 parts by weight; 0.5 to 3 parts by weight; 0.5 to 2 parts by weight; 1 to 3 parts by weight; or 2 to 4 parts by weight.
- the total amount of the first binder and the second binder is 0.5 to 4 parts by weight based on 100 parts by weight of the total mixture layer; 0.5 to 3 parts by weight; 0.5 to 2 parts by weight; 1 to 3 parts by weight; 2 to 5 parts by weight; Or it may be 1.5 to 2.5 parts by weight.
- the gap between the positive current collector and the first mixture layer and between the first mixture layer and the second mixture layer Adhesion can be easily improved.
- the positive electrode according to the present invention may contain a positive electrode additive represented by Formula 1 in at least one of the first mixture layer and the second mixture layer:
- M 1 is W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and At least one element selected from the group consisting of Mo,
- p and q are 5 ⁇ p ⁇ 7 and 0 ⁇ q ⁇ 0.5, respectively.
- the positive electrode additive contains excess lithium and can provide lithium for lithium consumption caused by irreversible chemical and physical reactions in the negative electrode during initial charging, thereby increasing the charging capacity of the battery and reducing the irreversible capacity, thereby improving lifespan characteristics this can be improved.
- the positive electrode additive represented by Chemical Formula 1 has a higher content of lithium ions than nickel-containing oxides commonly used in the art, so that lithium ions lost due to an irreversible reaction during initial activation of the battery can be supplemented, so that the charge and discharge of the battery capacity can be significantly improved.
- the lithium cobalt oxide represented by Chemical Formula 1 may include Li 6 CoO 4 , Li 6 Co 0.5 Zn 0.5 O 4 , Li 6 Co 0.7 Zn 0.3 O 4 , and the like.
- the average particle size of the lithium cobalt oxide represented by Formula 1 may be 0.1 to 10 ⁇ m, specifically 0.1 to 8 ⁇ m; 0.1 to 5 ⁇ m; 0.1 to 3 ⁇ m; 0.5 to 2 ⁇ m; 0.1 to 0.9 ⁇ m; 0.1 to 0.5 ⁇ m; 0.6 to 0.9 ⁇ m; 1 to 4 ⁇ m; 4 to 6 ⁇ m; Or it may be 6 to 9 ⁇ m.
- the average particle size of lithium cobalt oxide represented by Formula 1 may be 0.1 to 10 ⁇ m, specifically 0.1 to 8 ⁇ m; 0.1 to 5 ⁇ m; 0.1 to 3 ⁇ m; 0.5 to 2 ⁇ m; 0.1 to 0.9 ⁇ m; 0.1 to 0.5 ⁇ m; 0.6 to 0.9 ⁇ m; 1 to 4 ⁇ m; 4 to 6 ⁇ m; Or it may be 6 to 9 ⁇ m.
- the irreversible activity of lithium cobalt oxide can be increased and the powder electrical conductivity of lithium cobalt oxide can be prevented from being
- the lithium cobalt oxide represented by Chemical Formula 1 may have a tetragonal crystal structure, and may be included in a P4 2 /nmc space group having a twisted tetrahedral structure formed by a cobalt element and an oxygen element.
- Cathode additives having a twisted tetrahedral structure are structurally unstable due to the twisted tetrahedral structure formed by the cobalt element and oxygen atoms, and thus may be damaged by side reactions such as moisture (H 2 O) in the air during cathode manufacturing, and thus the electrical performance of the battery. this may deteriorate.
- the present invention can minimize damage to the positive electrode additive by using a binder having low affinity for water as a binder of the mixture layer, thereby further improving electrical performance and lifespan of the lithium secondary battery.
- the positive electrode additive may be included in an amount of 0.1 to 5 parts by weight, specifically 0.1 to 4 parts by weight, based on 100 parts by weight of each positive electrode mixture layer; 0.1 to 3 parts by weight; 0.1 to 2 parts by weight; 0.1 to 1 part by weight; 0.5 to 2 parts by weight; 1 to 3 parts by weight; 2 to 4 parts by weight; 1.5 to 3.5 parts by weight; 0.5 to 1.5 parts by weight; or 1 to 2 parts by weight.
- the positive electrode additive may be included in an amount of 0.1 to 0.5 parts by weight based on 100 parts by weight of the first mixture layer and 0.2 to 0.6 parts by weight based on 100 parts by weight of the second mixture layer.
- the positive electrode additive may be included only in the first mixture layer, and in this case, the amount included in the first mixture layer may be 0.5 to 2 parts by weight based on 100 parts by weight of the entire mixture layer.
- the first mixture layer may include a first cathode active material, a first conductive material, and a first binder
- the second mixture layer may include a second cathode active material, a second conductive material, and a second binder.
- the positive electrode additive may be included in any one of the first mixture layer and the second mixture layer.
- the first mixture layer includes a first cathode active material, a first conductive material, a cathode additive, and a first binder
- the second mixture layer includes a second cathode active material, a second conductive material, and a second binder.
- the present invention contains the positive electrode additive in the first mixture layer, thereby minimizing damage to the positive electrode additive caused by high temperature and/or high humidity during manufacturing of the positive electrode, thereby further improving the electrical performance and lifespan of the lithium secondary battery.
- the first cathode active material and the second cathode active material are nickel (Ni), cobalt (Co), manganese (Mn), aluminum (Al), zinc (Zn), titanium (Ti), magnesium (Mg), chromium ( It may be a lithium composite transition metal oxide containing two or more elements selected from the group consisting of Cr) and zirconium (Zr).
- the first positive electrode active material and the second positive electrode active material may each include a lithium metal composite oxide represented by Chemical Formula 2 capable of reversible intercalation and deintercalation:
- M 2 is W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and At least one element selected from the group consisting of Mo,
- x, y, z, w, v and u are 1.0 ⁇ x ⁇ 1.30, 0.1 ⁇ y ⁇ 0.95, 0.01 ⁇ z ⁇ 0.5, 0.01 ⁇ w ⁇ 0.5, 0 ⁇ v ⁇ 0.2, 1.5 ⁇ u ⁇ 4.5, respectively.
- the lithium metal composite oxide represented by Chemical Formula 2 is a composite metal oxide containing lithium, nickel, cobalt, and manganese, and may be doped with another transition metal (M 2 ) in some cases.
- the first positive electrode active material and the second positive electrode active material are LiNi 1/3 Co 1/3 Mn 1/3 O 2 , LiNi 0.6 Co 0.2 Mn 0.2 O 2 , LiNi 0.8 Co 0.1 Mn 0.1 O 2 , and LiNi 0.9 Co 0.05 Mn 0.05 O 2 , LiNi 0.8 Co 0.1 Mn 0.05 Al 0.05 O 2 , and LiNi 0.7 Co 0.1 Mn 0.1 Al 0.1 O 2 .
- the first positive electrode active material and the second positive electrode active material use LiNi 0.6 Co 0.2 Mn 0.2 O 2 and LiNi 0.8 Co 0.1 Mn 0.1 O 2 alone as lithium metal composite oxides represented by Chemical Formula 2, respectively, or can be combined
- first conductive material and the second conductive material may be used to improve performance such as electrical conductivity of the anode, and each of natural graphite, artificial graphite, carbon black, acetylene black, Ketjen black, carbon nanotubes, graphene and It may include one or more selected from the group consisting of carbon fibers.
- the content of the first conductive material and the second conductive material may be 0.5 to 5 parts by weight, specifically 0.5 to 4 parts by weight, based on 10 parts by weight of each mixture layer; 0.5 to 3 parts by weight; 0.5 to 1 part by weight; 0.5 to 2 parts by weight; 1 to 3 parts by weight; 2 to 4 parts by weight; 1.5 to 3.5 parts by weight; 0.5 to 1.5 parts by weight; Or it may be 1 to 2 parts by weight.
- the average thickness of the first mixture layer and the second mixture layer is not particularly limited, but is specifically 50 ⁇ m to 200 ⁇ m; 50 ⁇ m to 150 ⁇ m; 50 ⁇ m to 100 ⁇ m; 50 ⁇ m to 80 ⁇ m; 70 ⁇ m to 120 ⁇ m; Or it may be 60 ⁇ m to 110 ⁇ m.
- their total thickness may be 50 ⁇ m to 300 ⁇ m, more specifically 100 ⁇ m to 200 ⁇ m; 80 ⁇ m to 150 ⁇ m; 120 ⁇ m to 170 ⁇ m; 150 ⁇ m to 300 ⁇ m; 200 ⁇ m to 300 ⁇ m; Or it may be 150 ⁇ m to 190 ⁇ m.
- the positive electrode current collector one having high conductivity without causing chemical change in the battery may be used.
- stainless steel, aluminum, nickel, titanium, calcined carbon, etc. may be used, and aluminum or stainless steel may be surface-treated with carbon, nickel, titanium, silver, or the like.
- the positive electrode current collector may form fine irregularities on the surface to increase the adhesion of the positive electrode active material, and various forms such as films, sheets, foils, nets, porous bodies, foams, and nonwoven fabrics are possible.
- the average thickness of the positive electrode current collector may be appropriately applied in the range of 3 to 500 ⁇ m in consideration of the conductivity and total thickness of the positive electrode to be manufactured.
- a cathode for a lithium secondary battery containing a cathode additive represented by Formula 1 in at least one of the first mixture layer and the second mixture layer:
- M 1 is W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and At least one element selected from the group consisting of Mo,
- p and q are 5 ⁇ p ⁇ 7 and 0 ⁇ q ⁇ 0.5, respectively.
- the manufacturing method of a positive electrode for a lithium secondary battery according to the present invention may be performed through a process of forming a two-layered composite material layer on a positive electrode composite material layer. Specifically, the manufacturing method is performed by sequentially forming a first mixture layer and a second mixture layer on a positive electrode current collector, and the first binder layer and the second mixture layer have different affinity for water. and a second binder, respectively, and the positive electrode additive may be contained in at least one of the first mixture layer and the second mixture layer.
- the first mixture layer contains a first binder composed of a first cathode active material constituting the mixture layer, a cathode additive represented by Chemical Formula 1, a first conductive material, and a rubber-based resin at room temperature (eg, 22 ⁇ 3° C.) It may be prepared by dry mixing at a speed of 4000 rpm to prepare a composite material composition, and applying the prepared composite material composition to a positive electrode current collector.
- the process of drying the solvent can be omitted during the wet method, and thus productivity can be improved. movement can be prevented.
- the dry mixing method performed at a high speed of 1000 to 4000 rpm has an effect of uniformly coating the surface of each particle with the first binder, thereby improving the adhesion between particles and / or between the current collector and the composite layer.
- the cathode additive is included in the first mixture layer, it is possible to effectively prevent the cathode additive from being damaged due to moisture during manufacture of the cathode.
- the manufacturing method of the positive electrode for a lithium secondary battery includes a process of forming a second mixture layer on the formed first mixture layer, and in this case, the method of forming the second mixture layer may be applied without particular limitation.
- the second mixture layer may be formed by a wet method of forming a cathode slurry in which a second cathode active material, a second conductive material, a second binder, etc. are mixed in a solvent.
- usable solvents include N-methyl-2-pyrrolidone (NMP), dimethylacetamide (N,N-dimethyl acetamide, DMAc ), dimethylformamide (DMF), dimethyl sulfoxide (DMSO), acetonitrile (ACN), dimethylformamide (DMF)), acetone, and ethyl acetate.
- NMP N-methyl-2-pyrrolidone
- DMAc dimethylacetamide
- DMF dimethylformamide
- DMSO dimethyl sulfoxide
- ACN acetonitrile
- DMF dimethylformamide
- acetone and ethyl acetate.
- ethyl acetate may contain
- the solvents are used in a wet method, thereby minimizing damage to the positive electrode additive when the second mixture layer includes the positive electrode additive and uniformly forming the second positive electrode active material, the second conductive material, and the second binder. can mix well.
- drying of the positive electrode slurry applied on the positive electrode current collector may be performed at a temperature of 140° C. or lower in a vacuum state, specifically 130° C. or lower; below 120°C; below 110°C; below 100°C; below 80°C; below 70°C; below 60°C; below 50°C; below 40°C; 20° C. to 140° C.; 20° C. to 120° C.; 20° C. to 100° C.; 20° C. to 90° C.; 20° C. to 70° C.; 20° C. to 50° C.; 40° C. to 90° C.; 60° C. to 140° C.; 90° C. to 140° C.; Alternatively, it may be performed at 100 °C to 130 °C.
- the ratio of the amorphous phase to the crystalline phase of the fluorine-based resin, which is the second binder can be easily controlled to be as high as 51% or more by drying the positive electrode slurry under the above-described conditions.
- the method for manufacturing a positive electrode for a lithium secondary battery according to the present invention has the above configuration, thereby minimizing damage to the positive electrode additive and improving wettability to an electrolyte solution to improve the electrical performance of the battery. There is an advantage of improving the lifespan of the battery by improving the adhesion.
- a lithium secondary battery including a positive electrode, a negative electrode, and a separator interposed between the positive electrode and the negative electrode according to the present invention described above.
- the lithium secondary battery according to the present invention includes the above-described positive electrode of the present invention to further improve the adhesion between the positive electrode current collector and the composite layer, thereby improving the durability of the positive electrode and preventing damage to the positive electrode additive during manufacturing the positive electrode. Since it can be minimized, there is an advantage of further improving the electrical performance and lifespan of the lithium secondary battery.
- the lithium secondary battery of the present invention has a structure including a positive electrode, a negative electrode, and a separator interposed between the positive electrode and the negative electrode.
- the anode is manufactured by applying, drying, and pressing an anode active material on an anode current collector, and optionally may further include a conductive material, an organic binder polymer, and an additive, as in the cathode, as needed.
- the anode active material may include, for example, a carbon material and a silicon material.
- the carbon material refers to a carbon material containing carbon atoms as a main component, and examples of the carbon material include graphite having a completely layered crystal structure such as natural graphite, a low-crystalline graphene structure; a hexagonal honeycomb plane of carbon soft carbon having this layered structure) and hard carbon in which these structures are mixed with amorphous portions, artificial graphite, expanded graphite, carbon fiber, non-graphitizable carbon, carbon black, acetylene black, Ketjen black, carbon It may include nanotubes, fullerenes, activated carbon, graphene, carbon nanotubes, and the like, preferably at least one selected from the group consisting of natural graphite, artificial graphite, graphene, and carbon nanotubes.
- the carbon material includes natural graphite and/or artificial graphite, and may include at least one of graphene and carbon nanotubes together with the natural graphite and/or artificial graphite.
- the carbon material may include 50 to 95 parts by weight of graphene and/or carbon nanotubes based on 100 parts by weight of the total carbon material, and more specifically, 60 to 90 parts by weight based on 100 parts by weight of the total carbon material. wealth; Alternatively, 70 to 80 parts by weight of graphene and/or carbon nanotubes may be included.
- the silicon material is a particle containing silicon (Si) as a main component as a metal component, and may include at least one of a silicon (Si) particle and a silicon oxide (SiO X , 1 ⁇ X ⁇ 2) particle.
- the silicon material may include silicon (Si) particles, silicon monoxide (SiO) particles, silicon dioxide (SiO 2 ) particles, or a mixture of these particles.
- the silicon material may have a mixed form of crystalline particles and amorphous particles, and the ratio of the amorphous particles is 50 to 100 parts by weight, specifically 50 to 90 parts by weight, based on 100 parts by weight of the total silicon material; It may be 60 to 80 parts by weight or 85 to 100 parts by weight.
- the ratio of amorphous particles included in the silicon material within the above range, it is possible to improve thermal stability and flexibility of the electrode within a range that does not degrade electrical properties.
- the silicon material includes a carbon material and a silicon material, but may be included in an amount of 1 to 20 parts by weight based on 100 parts by weight of the negative electrode mixture layer, specifically, 5 to 20 parts by weight based on 100 parts by weight of the negative electrode mixture layer; 3 to 10 parts by weight; 8 to 15 parts by weight; 13 to 18 parts by weight; or 2 to 7 parts by weight.
- the present invention by adjusting the contents of the carbon material and the silicon material included in the negative electrode active material within the above ranges, it is possible to improve the charging capacity per unit mass while reducing lithium consumption and irreversible capacity loss during initial charging and discharging of the battery.
- the negative electrode active material may include 95 ⁇ 2 parts by weight of graphite based on 100 parts by weight of the negative electrode mixture layer; It may include 5 ⁇ 2 parts by weight of a mixture in which silicon monoxide (SiO) particles and silicon dioxide (SiO 2 ) particles are uniformly mixed.
- SiO silicon monoxide
- SiO 2 silicon dioxide
- the negative electrode mixture layer may have an average thickness of 100 ⁇ m to 200 ⁇ m, specifically, 100 ⁇ m to 180 ⁇ m, 100 ⁇ m to 150 ⁇ m, 120 ⁇ m to 200 ⁇ m, 140 ⁇ m to 200 ⁇ m, or 140 ⁇ m to 140 ⁇ m. It may have an average thickness of 160 ⁇ m.
- the anode current collector is not particularly limited as long as it does not cause chemical change in the battery and has high conductivity.
- copper, stainless steel, nickel, titanium, fired carbon, etc. may be used, and copper
- surface treatment with carbon, nickel, titanium, silver, etc. may be used.
- the negative electrode current collector may form fine irregularities on the surface to strengthen the bonding force with the negative electrode active material, and various forms such as films, sheets, foils, nets, porous bodies, foams, and nonwoven fabrics are available. It is possible.
- the average thickness of the negative electrode current collector may be appropriately applied in the range of 3 to 500 ⁇ m in consideration of the conductivity and total thickness of the negative electrode to be manufactured.
- the separator is interposed between the anode and the cathode, and an insulating thin film having high ion permeability and mechanical strength is used.
- the separator is not particularly limited as long as it is commonly used in the art, but specifically, chemical resistant and hydrophobic polypropylene; glass fiber; Alternatively, a sheet or non-woven fabric made of polyethylene may be used.
- a composite separator in which inorganic particles/organic particles are coated with an organic binder polymer may be used on a porous polymer substrate such as the sheet or non-woven fabric.
- the electrolyte may serve as a separator.
- the separator may have an average pore diameter of 0.01 to 10 ⁇ m and an average thickness of 5 to 300 ⁇ m.
- the positive and negative electrodes may be rolled in a jelly roll form and stored in a cylindrical battery, prismatic battery, or pouch type battery, or may be stored in a pouch type battery in a folding or stack-and-folding form, but are not limited thereto.
- the lithium salt-containing electrolyte solution according to the present invention may be composed of an electrolyte solution and a lithium salt, and a non-aqueous organic solvent, an organic solid electrolyte, an inorganic solid electrolyte, or the like may be used as the electrolyte solution.
- non-aqueous organic solvent for example, N-methyl-2-pyrrolidinone, ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, gamma-butyrolactone, 1,2-dimethine Toxy ethane, tetrahydroxy franc, 2-methyl tetrahydrofuran, dimethyl sulfoxide, 1,3-dioxorane, formamide, dimethylformamide, dioxorane, acetonitrile, nitromethane, methyl formate, Methyl acetate, phosphoric acid triesters, trimethoxy methane, dioxolane derivatives, sulfolane, methyl sulfolane, 1,3-dimethyl-2-imidazolidinone, propylene carbonate derivatives, tetrahydrofuran derivatives, ether, propion An aprotic organic solvent such as methyl acid or ethyl propyl
- organic solid electrolyte examples include polyethylene derivatives, polyethylene oxide derivatives, polypropylene oxide derivatives, phosphoric acid ester polymers, poly agitation lysine, polyester sulfide, polyvinyl alcohol, polyvinylidene fluoride, ions
- a polymeric material containing a sexual dissociation group or the like can be used.
- Examples of the inorganic solid electrolyte include Li 3 N, LiI, Li 5 Ni 2 , Li 3 N-LiI-LiOH, LiSiO 4 , LiSiO 4 -LiI-LiOH, Li 2 SiS 3 , Li 4 SiO 4 , Nitride, halide, sulfate, and the like of Li such as Li 4 SiO 4 -LiI-LiOH, Li 3 PO 4 -Li 2 S-SiS 2 , etc. may be used.
- the lithium salt is a material that is easily soluble in non-aqueous electrolytes, for example, LiCl, LiBr, LiI, LiClO 4 , LiBF 4 , LiB10Cl 10 , LiPF 6 , LiCF 3 SO 3 , LiCF 3 CO 2 , LiAsF 6 , LiSbF 6 , LiAlCl 4 , CH 3 SO 3 Li, (CF 3 SO 2 ) 2 NLi, lithium chloroborane, lithium lower aliphatic carboxylic acid, lithium 4-phenylborate, imide and the like can be used.
- LiCl, LiBr, LiI, LiClO 4 , LiBF 4 , LiB10Cl 10 LiPF 6 , LiCF 3 SO 3 , LiCF 3 CO 2 , LiAsF 6 , LiSbF 6 , LiAlCl 4 , CH 3 SO 3 Li, (CF 3 SO 2 ) 2 NLi, lithium chloroborane, lithium lower aliphatic carb
- pyridine triethylphosphite, triethanolamine, cyclic ether, ethylene diamine, n-glyme, hexaphosphoric acid triamide, nitro Benzene derivatives, sulfur, quinone imine dyes, N-substituted oxazolidinones, N,N-substituted imidazolidines, ethylene glycol dialkyl ethers, ammonium salts, pyrrole, 2-methoxy ethanol, aluminum trichloride, etc. may be added.
- pyridine triethylphosphite, triethanolamine, cyclic ether, ethylene diamine, n-glyme, hexaphosphoric acid triamide, nitro Benzene derivatives, sulfur, quinone imine dyes, N-substituted oxazolidinones, N,N-substituted imidazolidines, ethylene glycol dialkyl ethers, ammonium salts
- halogen-containing solvents such as carbon tetrachloride and ethylene trifluoride may be further included to impart incombustibility, and carbon dioxide gas may be further included to improve storage properties at high temperatures.
- FEC Fluoro-Ethylene Carbonate
- PRS Pene sultone
- N-methylpyrrolidone was injected into a homo mixer, and LiNi 0.6 Co 0.2 Mn 0.2 O 2 (average particle size: 1 ⁇ 0.5 ⁇ m) as a second cathode active material based on 100 parts by weight of the solid content of the cathode slurry 48.5 parts by weight; 0.5 parts by weight of carbon black (average particle size: 2 ⁇ 0.5 ⁇ m) as a second conductive material; 1 part by weight of polyvinylidene fluoride (PVdF) as a second binder was weighed and added, and mixed at room temperature at 2,000 ⁇ 500 rpm for 50 to 70 minutes to prepare a positive electrode slurry.
- PVdF polyvinylidene fluoride
- a previously prepared mixture composition was applied to one surface of the aluminum current collector and passed through hot-press rollers to form a rolled first mixture layer.
- the positive electrode slurry was continuously applied on the first mixture layer, vacuum dried under the temperature conditions shown in Table 1 below, and then rolled to prepare a positive electrode for a lithium secondary battery.
- the thicknesses of the first mixture layer and the second mixture layer were 55 ⁇ m and 80 ⁇ m, respectively, and the total thickness of the manufactured positive electrode was about 200 ⁇ m.
- Example 1 Example 2 Example 3 Comparative Example 1 Comparative Example 2 Second mixture layer drying temperature 40 ⁇ 5°C 70 ⁇ 5°C 130 ⁇ 5°C 150 ⁇ 5°C 180 ⁇ 5°C
- PVdF polyvinylidene fluoride
- a positive electrode was fabricated in the same manner as in Examples 1 to 3 and Comparative Examples 1 to 3, but the static water contact angle with respect to the surface of each mixture layer was measured when the first mixture layer and the second mixture layer were respectively formed.
- the static water contact angle was measured by a sessile drop method. Specifically, it is performed by dropping one drop of purified water on the surface of each mixture layer, capturing an image of the dropped liquid drop, and then analyzing the captured image.
- the positive electrodes prepared in Examples 1 to 3 and Comparative Examples 1 to 3 were cut to have horizontal and vertical lengths of 25 mm and 70 mm, respectively, and were laminated using a press at 70 ° C. and 4 MPa to prepare specimens.
- the prepared specimen was attached and fixed to a glass plate using double-sided tape, and at this time, the positive electrode current collector was placed facing the glass plate.
- the membrane portion of the specimen was peeled at an angle of 90° at a speed of 100 mm/min at 25 °C, and the peel force at this time was measured in real time, and the average value was determined as the interfacial adhesive force between the first and second mixture layers. defined; Subsequently, the same method was continuously performed to measure the interfacial adhesion between the positive electrode current collector and the first mixture layer.
- Table 2 The results are shown in Table 2 below.
- a negative electrode slurry was prepared by preparing 2 parts by weight of styrene butadiene rubber (SBR) as a binder and performing the same method as preparing the positive electrode slurry.
- the graphite used in preparing the negative electrode mixture layer was natural graphite (average particle size: 0.01 to 0.5 ⁇ m), and silicon (SiOx) particles having an average particle size of 0.9 to 1.1 ⁇ m were used.
- the prepared anode slurry was coated on one surface of a copper current collector, dried at 100° C., and rolled to prepare a cathode. At this time, the total thickness of the negative electrode mixture layer was 150 ⁇ m, and the total thickness of the prepared negative electrode was about 250 ⁇ m.
- a separator made of a porous polyethylene (PE) film (thickness: about 16 ⁇ m) was laminated between the positive electrode and the negative electrode prepared in Examples 1 to 3 and Comparative Examples 1 to 3, and E2DVC was injected as an electrolyte to form a full cell (full cell).
- a cell type lithium secondary battery was manufactured.
- E2DVC is a kind of carbonate-based electrolyte
- the manufactured lithium secondary battery was charged at a temperature of 25 ° C with a charging current of 0.1 C to a charging end voltage of 4.2 to 4.25 V, and then charged until the current density reached 0.01 C at the end voltage. Thereafter, the battery was discharged to a final voltage of 2V with a discharge current of 0.1C, and the initial charge/discharge capacity per unit mass was measured. The results are shown in Table 2 below.
- the positive electrode for a lithium secondary battery according to the present invention has excellent adhesion between the positive electrode current collector and the positive electrode mixture layer, and has a high charging capacity of the battery.
- the positive electrodes for lithium secondary batteries contain a rubber-based resin and a fluorine-based resin as binders in the first mixture layer and the second mixture layer, respectively, so that the affinity for water of each mixture layer is controlled. It was found that the mixture layer had a lower affinity for water, so that the static water contact angle deviation (A-B) between the first mixture layer (A) and the second mixture layer (B) had a difference of 5° or more.
- the positive electrode for a lithium secondary battery according to the present invention has a structure in which a positive electrode current collector, a first mixture layer, and a second mixture layer are sequentially stacked, and a binder that is more hydrophobic than the binder contained in the second mixture layer is used as a positive electrode.
- the adhesion between the positive electrode current collector and the composite layer can be further improved, so that the durability of the positive electrode can be improved, and when the first mixture layer contains the positive electrode additive, water It can be seen that the electrical performance and lifespan of the lithium secondary battery can be further improved because damage to the positive electrode additive can be minimized during the manufacture of the positive electrode due to the first binder having a low affinity for the first binder.
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Abstract
Description
실시예 1 | 실시예 2 | 실시예 3 | 비교예 1 | 비교예 2 | |
제2 합재층건조 온도 | 40±5℃ | 70±5℃ | 130±5℃ | 150±5℃ | 180±5℃ |
정적 물 접촉각 | 계면 접착력 [N/m] | 초기 충전용량 |
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제1 합재층 (A) |
제2 합재층 (B) |
A-B | 집전체-제1 합재층 | 제1 합재층-제2 합재층 | ||
실시예 1 | 143° | 110° | 33° | 408 | 38 | 103.8 |
실시예 2 | 142° | 114° | 28° | 413 | 39 | 104.7 |
실시예 3 | 144° | 134° | 10° | 402 | 37 | 104.2 |
비교예 1 | 141° | 137° | 4° | 374 | 24 | 101.5 |
비교예 2 | 143° | 144° | -1° | 361 | 25 | 100.2 |
비교예 3 | 146° | 146° | 0° | 320 | 14 | 101.6 |
Claims (16)
- 양극 집전체, 제1 합재층 및 제2 합재층이 순차적으로 적층된 구조를 가지며;상기 제1 합재층은 고무계 수지로 구성된 제1 바인더를 포함하고,상기 제2 합재층은 불소(F) 함유 단량체로부터 유래되는 불소계 수지로 구성된 제2 바인더를 포함하는 리튬 이차전지용 양극.
- 제1항에 있어서,제1 합재층의 정적 물 접촉각은 제2 합재층의 정적 물 접촉각보다 5° 이상 큰 것을 특징으로 하는 리튬 이차전지용 양극.
- 제1항에 있어서,제1 합재층의 정적 물 접촉각은 제2 합재층의 정적 물 접촉각보다 10° 내지 30° 큰 것을 특징으로 하는 리튬 이차전지용 양극.
- 제1항에 있어서,고무계 수지는 스티렌-부타디엔 고무, 니트릴-부타디엔 고무, 메틸메타크릴레이트-부타디엔 고무, 클로로프렌 고무, 카르복시 변성 스티렌 부타디엔 고무, 및 변성 폴리오가노실록산 중합체로 이루어진 군으로부터 선택된 1종 이상을 포함하는 리튬 이차전지용 양극.
- 제1항에 있어서,불소계 수지는 비닐리덴 플루오라이드(VDF 또는 VF2), 테트라플루오로에틸렌(TFE), 트리플루오로에틸렌(TrFE), 클로로트리플루오로에틸렌(CTFE), 헥사플루오로프로펜(HFP), 비닐 플루오라이드(VF), 헥사플루오로이소부틸렌(HFIB), 퍼플루오로부틸에틸렌(PFBE), 펜타플루오로프로펜, 3,3,3-트리플루오로-1-프로펜 및 2-트리플루오로메틸-3,3,3-트리플루오로프로펜으로 이루어진 군으로부터 선택되는 1종 이상의 단량체로부터 유래되는 수지를 포함하는 리튬 이차전지용 양극.
- 제1항에 있어서,제1 바인더의 함량은 제1 합재층 100 중량부에 대하여 0.5 내지 5 중량부이고,제2 바인더의 함량은 제2 합재층 100 중량부에 대하여 0.5 내지 10 중량부이되,제1 바인더 및 제2 바인더의 총 함량은 전체 합재층 100 중량부에 대하여 0.1 내지 5 중량부인 리튬 이차전지용 양극.
- 제1항에 있어서,상기 제1 합재층 및 제2 합재층 중 어느 하나 이상의 합재층에 하기 화학식 1로 나타내는 양극 첨가제를 함유하는 리튬 이차전지용 양극:[화학식 1]LipCo(1-q)M1 qO4상기 화학식 1에서,M1은 W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, 및 Mo로 이루어진 군에서 선택되는 1종 이상의 원소이고,p 및 q는 각각 5≤p≤7 및 0≤q≤0.5이다.
- 제7항에 있어서,양극 첨가제는 각 양극 합재층 100 중량부에 대하여 0.1 내지 5 중량부로 포함되는 리튬 이차전지용 양극.
- 제7항에 있어서,양극 첨가제는 공간군이 P42/nmc인 정방정계 구조(tetragonal structure)를 갖는 리튬 이차전지용 양극.
- 제1항에 있어서,제1 합재층은 제1 양극활물질, 제1 도전재, 양극 첨가제 및 제1 바인더를 포함하고,제2 합재층은 제2 양극활물질, 제2 도전재 및 제2 바인더를 포함하는 리튬 이차전지용 양극.
- 제10항에 있어서,제1 양극활물질 및 제2 양극활물질은 각각 하기 화학식 2로 나타내는 리튬 금속 복합 산화물을 포함하는 리튬 이차전지용 양극:[화학식 2]Lix[NiyCozMnwM2 v]Ou상기 화학식 2에 있어서,M2는 W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, 및 Mo로 이루어진 군에서 선택되는 1종 이상의 원소이고,x, y, z, w, v 및 u는 각각 1.0≤x≤1.30, 0.1≤y<0.95, 0.01<z≤0.5, 0.01<w≤0.5, 0≤v≤0.2, 1.5≤u≤4.5이다.
- 제10항에 있어서,제1 도전재 및 제2 도전재는 각각 천연 흑연, 인조 흑연, 카본 블랙, 아세틸렌 블랙, 케첸 블랙, 탄소나노튜브, 그래핀 및 탄소섬유로 이루어진 군으로부터 선택되는 1종 이상을 포함하는 리튬 이차전지용 양극.
- 제10항에 있어서,제1 도전재 및 제2 도전재의 함량은 각각 양극 합재층 100 중량부에 대하여 0.5 내지 5 중량부인 리튬 이차전지용 양극.
- 양극 합재층 상에 고무계 수지로 구성된 제1 바인더를 함유하는 제1 합재층을 형성하는 단계; 및제1 합재층 상에 불소(F) 함유 단량체로부터 유래되는 불소계 수지로 구성된 제2 바인더를 함유하는 제2 합재층을 형성하는 단계를 포함하는 리튬 이차전지용 양극의 제조방법.
- 제14항에 있어서,상기 제1 합재층 및 제2 합재층 중 어느 하나 이상의 합재층에 하기 화학식 1로 나타내는 양극 첨가제를 함유하는 리튬 이차전지용 양극의 제조방법:[화학식 1]LipCo(1-q)M1 qO4상기 화학식 1에서,M1은 W, Cu, Fe, V, Cr, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, 및 Mo로 이루어진 군에서 선택되는 1종 이상의 원소이고,p 및 q는 각각 5≤p≤7 및 0≤q≤0.5이다.
- 제14항에 있어서,제1 합재층을 형성하는 단계는,제1 양극활물질, 화학식 1로 나타내는 양극 첨가제, 제1 도전재 및 고무계 수지로 구성된 제1 바인더를 건식 혼합하여 합재 조성물을 제조하는 단계; 및제조된 합재 조성물을 양극 집전체 상에 도포하는 단계를 통해 수행되는 리튬 이차전지용 양극의 제조방법.
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- 2022-05-06 CN CN202280006366.2A patent/CN116057725A/zh active Pending
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