US20200235378A1 - Positive active material - Google Patents
Positive active material Download PDFInfo
- Publication number
- US20200235378A1 US20200235378A1 US16/843,455 US202016843455A US2020235378A1 US 20200235378 A1 US20200235378 A1 US 20200235378A1 US 202016843455 A US202016843455 A US 202016843455A US 2020235378 A1 US2020235378 A1 US 2020235378A1
- Authority
- US
- United States
- Prior art keywords
- active material
- positive active
- core
- compound
- stabilizing compound
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Abandoned
Links
- 239000007774 positive electrode material Substances 0.000 title claims abstract description 114
- 150000001875 compounds Chemical class 0.000 claims abstract description 125
- 239000000126 substance Substances 0.000 claims abstract description 25
- 229910052748 manganese Inorganic materials 0.000 claims abstract description 9
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 8
- 229910052749 magnesium Inorganic materials 0.000 claims abstract description 7
- 229910052796 boron Inorganic materials 0.000 claims abstract description 6
- 229910052750 molybdenum Inorganic materials 0.000 claims abstract description 6
- 229910052698 phosphorus Inorganic materials 0.000 claims abstract description 6
- 229910052719 titanium Inorganic materials 0.000 claims abstract description 6
- 229910052720 vanadium Inorganic materials 0.000 claims abstract description 6
- 229910052727 yttrium Inorganic materials 0.000 claims abstract description 6
- 229910052726 zirconium Inorganic materials 0.000 claims abstract description 6
- 229910052788 barium Inorganic materials 0.000 claims abstract description 5
- 229910052746 lanthanum Inorganic materials 0.000 claims abstract description 5
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 5
- 229910052721 tungsten Inorganic materials 0.000 claims abstract description 5
- 238000000034 method Methods 0.000 claims description 57
- 229910009998 LiaCoO2 Inorganic materials 0.000 claims description 27
- 239000000203 mixture Substances 0.000 claims description 27
- UBEWDCMIDFGDOO-UHFFFAOYSA-N cobalt(II,III) oxide Inorganic materials [O-2].[O-2].[O-2].[O-2].[Co+2].[Co+3].[Co+3] UBEWDCMIDFGDOO-UHFFFAOYSA-N 0.000 claims description 24
- 238000002156 mixing Methods 0.000 claims description 23
- 229910021503 Cobalt(II) hydroxide Inorganic materials 0.000 claims description 16
- 239000002904 solvent Substances 0.000 claims description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 10
- 229910052760 oxygen Inorganic materials 0.000 claims description 10
- 239000001301 oxygen Substances 0.000 claims description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 4
- 229910052744 lithium Inorganic materials 0.000 abstract description 43
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 abstract description 35
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 43
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 33
- 239000003792 electrolyte Substances 0.000 description 21
- 239000007773 negative electrode material Substances 0.000 description 20
- 239000011572 manganese Substances 0.000 description 18
- -1 Co(OH)3 Inorganic materials 0.000 description 16
- 239000004020 conductor Substances 0.000 description 16
- 238000004519 manufacturing process Methods 0.000 description 16
- 230000000052 comparative effect Effects 0.000 description 14
- 229910052759 nickel Inorganic materials 0.000 description 14
- 239000011230 binding agent Substances 0.000 description 13
- 229910000361 cobalt sulfate Inorganic materials 0.000 description 13
- 229940044175 cobalt sulfate Drugs 0.000 description 13
- KTVIXTQDYHMGHF-UHFFFAOYSA-L cobalt(2+) sulfate Chemical compound [Co+2].[O-]S([O-])(=O)=O KTVIXTQDYHMGHF-UHFFFAOYSA-L 0.000 description 13
- LGQLOGILCSXPEA-UHFFFAOYSA-L nickel sulfate Chemical compound [Ni+2].[O-]S([O-])(=O)=O LGQLOGILCSXPEA-UHFFFAOYSA-L 0.000 description 13
- 229910000363 nickel(II) sulfate Inorganic materials 0.000 description 13
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 12
- 229910001416 lithium ion Inorganic materials 0.000 description 12
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 11
- 229910052731 fluorine Inorganic materials 0.000 description 11
- 239000011737 fluorine Substances 0.000 description 11
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 9
- 239000013078 crystal Substances 0.000 description 9
- 239000002243 precursor Substances 0.000 description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 7
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 7
- 239000004698 Polyethylene Substances 0.000 description 7
- 239000004743 Polypropylene Substances 0.000 description 7
- DIZPMCHEQGEION-UHFFFAOYSA-H aluminium sulfate (anhydrous) Chemical compound [Al+3].[Al+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O DIZPMCHEQGEION-UHFFFAOYSA-H 0.000 description 7
- 230000015572 biosynthetic process Effects 0.000 description 7
- 239000003575 carbonaceous material Substances 0.000 description 7
- 229920000573 polyethylene Polymers 0.000 description 7
- 229920001155 polypropylene Polymers 0.000 description 7
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 6
- 229910001290 LiPF6 Inorganic materials 0.000 description 6
- 239000002033 PVDF binder Substances 0.000 description 6
- 238000000576 coating method Methods 0.000 description 6
- 239000000463 material Substances 0.000 description 6
- 239000003960 organic solvent Substances 0.000 description 6
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 5
- 150000004945 aromatic hydrocarbons Chemical class 0.000 description 5
- 229910021383 artificial graphite Inorganic materials 0.000 description 5
- 239000003660 carbonate based solvent Substances 0.000 description 5
- 125000004093 cyano group Chemical group *C#N 0.000 description 5
- 238000011156 evaluation Methods 0.000 description 5
- 238000007429 general method Methods 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 239000003273 ketjen black Substances 0.000 description 5
- 229910003002 lithium salt Inorganic materials 0.000 description 5
- 159000000002 lithium salts Chemical class 0.000 description 5
- 229940099596 manganese sulfate Drugs 0.000 description 5
- 235000007079 manganese sulphate Nutrition 0.000 description 5
- 239000011702 manganese sulphate Substances 0.000 description 5
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 5
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- 239000012046 mixed solvent Substances 0.000 description 5
- 229910021382 natural graphite Inorganic materials 0.000 description 5
- 229940053662 nickel sulfate Drugs 0.000 description 5
- 239000010936 titanium Substances 0.000 description 5
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 4
- 229910052783 alkali metal Inorganic materials 0.000 description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 4
- 229910052802 copper Inorganic materials 0.000 description 4
- 239000010949 copper Substances 0.000 description 4
- 229910052593 corundum Inorganic materials 0.000 description 4
- 125000000449 nitro group Chemical group [O-][N+](*)=O 0.000 description 4
- 229910001845 yogo sapphire Inorganic materials 0.000 description 4
- PBKONEOXTCPAFI-UHFFFAOYSA-N 1,2,4-trichlorobenzene Chemical compound ClC1=CC=C(Cl)C(Cl)=C1 PBKONEOXTCPAFI-UHFFFAOYSA-N 0.000 description 3
- RFFLAFLAYFXFSW-UHFFFAOYSA-N 1,2-dichlorobenzene Chemical compound ClC1=CC=CC=C1Cl RFFLAFLAYFXFSW-UHFFFAOYSA-N 0.000 description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 3
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 3
- 229910002651 NO3 Inorganic materials 0.000 description 3
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- 150000001340 alkali metals Chemical class 0.000 description 3
- 229910045601 alloy Inorganic materials 0.000 description 3
- 239000000956 alloy Substances 0.000 description 3
- 229910017052 cobalt Inorganic materials 0.000 description 3
- 239000010941 cobalt Substances 0.000 description 3
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 3
- 229920001971 elastomer Polymers 0.000 description 3
- 239000000835 fiber Substances 0.000 description 3
- 229910052736 halogen Inorganic materials 0.000 description 3
- 150000002367 halogens Chemical class 0.000 description 3
- 229910021385 hard carbon Inorganic materials 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 3
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 3
- 229910052808 lithium carbonate Inorganic materials 0.000 description 3
- 229940006116 lithium hydroxide Drugs 0.000 description 3
- 239000011356 non-aqueous organic solvent Substances 0.000 description 3
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 3
- 239000005060 rubber Substances 0.000 description 3
- 229910052709 silver Inorganic materials 0.000 description 3
- 229920003048 styrene butadiene rubber Polymers 0.000 description 3
- 239000003232 water-soluble binding agent Substances 0.000 description 3
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 description 2
- GOYDNIKZWGIXJT-UHFFFAOYSA-N 1,2-difluorobenzene Chemical compound FC1=CC=CC=C1F GOYDNIKZWGIXJT-UHFFFAOYSA-N 0.000 description 2
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
- OZJPLYNZGCXSJM-UHFFFAOYSA-N 5-valerolactone Chemical compound O=C1CCCCO1 OZJPLYNZGCXSJM-UHFFFAOYSA-N 0.000 description 2
- 229920000049 Carbon (fiber) Polymers 0.000 description 2
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 2
- 229910032387 LiCoO2 Inorganic materials 0.000 description 2
- 229910014063 LiNi1-xCoxO2 Inorganic materials 0.000 description 2
- 229910014402 LiNi1—xCoxO2 Inorganic materials 0.000 description 2
- 229910002097 Lithium manganese(III,IV) oxide Inorganic materials 0.000 description 2
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 2
- 229920000265 Polyparaphenylene Polymers 0.000 description 2
- 239000004372 Polyvinyl alcohol Substances 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 2
- 239000006230 acetylene black Substances 0.000 description 2
- 229920005993 acrylate styrene-butadiene rubber polymer Polymers 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 230000000996 additive effect Effects 0.000 description 2
- 239000005456 alcohol based solvent Substances 0.000 description 2
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 2
- 150000001342 alkaline earth metals Chemical class 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 229910021502 aluminium hydroxide Inorganic materials 0.000 description 2
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 2
- 229910003481 amorphous carbon Inorganic materials 0.000 description 2
- 239000000010 aprotic solvent Substances 0.000 description 2
- 229910052795 boron group element Inorganic materials 0.000 description 2
- 229910052791 calcium Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 239000004917 carbon fiber Substances 0.000 description 2
- 229910052800 carbon group element Inorganic materials 0.000 description 2
- 239000001768 carboxy methyl cellulose Substances 0.000 description 2
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 2
- 239000005466 carboxylated polyvinylchloride Substances 0.000 description 2
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 2
- 239000001913 cellulose Substances 0.000 description 2
- 229920002678 cellulose Polymers 0.000 description 2
- 229910052798 chalcogen Inorganic materials 0.000 description 2
- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 description 2
- 229920001940 conductive polymer Polymers 0.000 description 2
- 229920001577 copolymer Polymers 0.000 description 2
- 150000005676 cyclic carbonates Chemical class 0.000 description 2
- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 2
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000003822 epoxy resin Substances 0.000 description 2
- 239000003759 ester based solvent Substances 0.000 description 2
- 235000019441 ethanol Nutrition 0.000 description 2
- 239000004210 ether based solvent Substances 0.000 description 2
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 2
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 description 2
- QKBJDEGZZJWPJA-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound [CH2]COC(=O)OCCC QKBJDEGZZJWPJA-UHFFFAOYSA-N 0.000 description 2
- 125000003709 fluoroalkyl group Chemical group 0.000 description 2
- 239000006260 foam Substances 0.000 description 2
- 229910001679 gibbsite Inorganic materials 0.000 description 2
- 150000002431 hydrogen Chemical class 0.000 description 2
- 229910052738 indium Inorganic materials 0.000 description 2
- 238000009830 intercalation Methods 0.000 description 2
- 239000005453 ketone based solvent Substances 0.000 description 2
- 229910052745 lead Inorganic materials 0.000 description 2
- XIXADJRWDQXREU-UHFFFAOYSA-M lithium acetate Chemical compound [Li+].CC([O-])=O XIXADJRWDQXREU-UHFFFAOYSA-M 0.000 description 2
- 229940008015 lithium carbonate Drugs 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- IIPYXGDZVMZOAP-UHFFFAOYSA-N lithium nitrate Chemical compound [Li+].[O-][N+]([O-])=O IIPYXGDZVMZOAP-UHFFFAOYSA-N 0.000 description 2
- 230000014759 maintenance of location Effects 0.000 description 2
- 239000007769 metal material Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 description 2
- 239000003235 non-water-soluble binding agent Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 229910052696 pnictogen Inorganic materials 0.000 description 2
- 229920000647 polyepoxide Polymers 0.000 description 2
- 239000002952 polymeric resin Substances 0.000 description 2
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 2
- 239000004810 polytetrafluoroethylene Substances 0.000 description 2
- 229920002635 polyurethane Polymers 0.000 description 2
- 239000004814 polyurethane Substances 0.000 description 2
- 229920002451 polyvinyl alcohol Polymers 0.000 description 2
- 229920000915 polyvinyl chloride Polymers 0.000 description 2
- 239000004800 polyvinyl chloride Substances 0.000 description 2
- 229920002620 polyvinyl fluoride Polymers 0.000 description 2
- 229920000973 polyvinylchloride carboxylated Polymers 0.000 description 2
- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 2
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 2
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 description 2
- 229910052700 potassium Inorganic materials 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- YKYONYBAUNKHLG-UHFFFAOYSA-N propyl acetate Chemical compound CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- 229910052708 sodium Inorganic materials 0.000 description 2
- 230000000087 stabilizing effect Effects 0.000 description 2
- 229910052712 strontium Inorganic materials 0.000 description 2
- 229920003002 synthetic resin Polymers 0.000 description 2
- 239000002562 thickening agent Substances 0.000 description 2
- 229910052718 tin Inorganic materials 0.000 description 2
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 2
- 230000007704 transition Effects 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 229910000314 transition metal oxide Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- 229910052725 zinc Inorganic materials 0.000 description 2
- JYVXNLLUYHCIIH-UHFFFAOYSA-N (+/-)-mevalonolactone Natural products CC1(O)CCOC(=O)C1 JYVXNLLUYHCIIH-UHFFFAOYSA-N 0.000 description 1
- LNAZSHAWQACDHT-XIYTZBAFSA-N (2r,3r,4s,5r,6s)-4,5-dimethoxy-2-(methoxymethyl)-3-[(2s,3r,4s,5r,6r)-3,4,5-trimethoxy-6-(methoxymethyl)oxan-2-yl]oxy-6-[(2r,3r,4s,5r,6r)-4,5,6-trimethoxy-2-(methoxymethyl)oxan-3-yl]oxyoxane Chemical compound CO[C@@H]1[C@@H](OC)[C@H](OC)[C@@H](COC)O[C@H]1O[C@H]1[C@H](OC)[C@@H](OC)[C@H](O[C@H]2[C@@H]([C@@H](OC)[C@H](OC)O[C@@H]2COC)OC)O[C@@H]1COC LNAZSHAWQACDHT-XIYTZBAFSA-N 0.000 description 1
- 125000000008 (C1-C10) alkyl group Chemical group 0.000 description 1
- LHOGNQZQKDZOBP-UHFFFAOYSA-N 1,2,3-trichloro-4-methylbenzene Chemical compound CC1=CC=C(Cl)C(Cl)=C1Cl LHOGNQZQKDZOBP-UHFFFAOYSA-N 0.000 description 1
- RELMFMZEBKVZJC-UHFFFAOYSA-N 1,2,3-trichlorobenzene Chemical compound ClC1=CC=CC(Cl)=C1Cl RELMFMZEBKVZJC-UHFFFAOYSA-N 0.000 description 1
- LRQPEHJWTXCLQY-UHFFFAOYSA-N 1,2,3-trifluoro-4-methylbenzene Chemical compound CC1=CC=C(F)C(F)=C1F LRQPEHJWTXCLQY-UHFFFAOYSA-N 0.000 description 1
- AJKNNUJQFALRIK-UHFFFAOYSA-N 1,2,3-trifluorobenzene Chemical compound FC1=CC=CC(F)=C1F AJKNNUJQFALRIK-UHFFFAOYSA-N 0.000 description 1
- HXDPORRJTJUJIF-UHFFFAOYSA-N 1,2,3-triiodo-4-methylbenzene Chemical compound CC1=CC=C(I)C(I)=C1I HXDPORRJTJUJIF-UHFFFAOYSA-N 0.000 description 1
- RIWAPWDHHMWTRA-UHFFFAOYSA-N 1,2,3-triiodobenzene Chemical compound IC1=CC=CC(I)=C1I RIWAPWDHHMWTRA-UHFFFAOYSA-N 0.000 description 1
- PEBWOGPSYUIOBP-UHFFFAOYSA-N 1,2,4-trifluorobenzene Chemical compound FC1=CC=C(F)C(F)=C1 PEBWOGPSYUIOBP-UHFFFAOYSA-N 0.000 description 1
- KSXFNGRHPAHIQJ-UHFFFAOYSA-N 1,2,4-triiodobenzene Chemical compound IC1=CC=C(I)C(I)=C1 KSXFNGRHPAHIQJ-UHFFFAOYSA-N 0.000 description 1
- OKLGPXYADUOPGA-UHFFFAOYSA-N 1,2,5-trichloro-3-methylbenzene Chemical compound CC1=CC(Cl)=CC(Cl)=C1Cl OKLGPXYADUOPGA-UHFFFAOYSA-N 0.000 description 1
- ZQWBCGBMUFLFPC-UHFFFAOYSA-N 1,2,5-trifluoro-3-methylbenzene Chemical compound CC1=CC(F)=CC(F)=C1F ZQWBCGBMUFLFPC-UHFFFAOYSA-N 0.000 description 1
- YMZNUPTUGITAHW-UHFFFAOYSA-N 1,2,5-triiodo-3-methylbenzene Chemical compound CC1=CC(I)=CC(I)=C1I YMZNUPTUGITAHW-UHFFFAOYSA-N 0.000 description 1
- GWLKCPXYBLCEKC-UHFFFAOYSA-N 1,2-dichloro-3-methylbenzene Chemical compound CC1=CC=CC(Cl)=C1Cl GWLKCPXYBLCEKC-UHFFFAOYSA-N 0.000 description 1
- ZNEHIDGAPGVZSA-UHFFFAOYSA-N 1,2-difluoro-3-methylbenzene Chemical compound CC1=CC=CC(F)=C1F ZNEHIDGAPGVZSA-UHFFFAOYSA-N 0.000 description 1
- PFLNKRGFZQUABS-UHFFFAOYSA-N 1,2-diiodo-3-methylbenzene Chemical compound CC1=CC=CC(I)=C1I PFLNKRGFZQUABS-UHFFFAOYSA-N 0.000 description 1
- BBOLNFYSRZVALD-UHFFFAOYSA-N 1,2-diiodobenzene Chemical compound IC1=CC=CC=C1I BBOLNFYSRZVALD-UHFFFAOYSA-N 0.000 description 1
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Images
Classifications
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- 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
- 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
- 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
- H01M4/13—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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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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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
- H01M4/362—Composites
- H01M4/366—Composites as layered products
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- H—ELECTRICITY
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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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
-
- 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
- Embodiments are directed to a positive active material for a rechargeable lithium battery and a rechargeable lithium battery including the same.
- a rechargeable lithium battery may be used as an actuating power source for a mobile information terminal such as a cell phone, a laptop, a smart phone, and the like.
- the rechargeable lithium battery includes a positive electrode, a negative electrode, and an electrolyte.
- a positive active material of a positive electrode may be an oxide consisting of lithium and a transition metal and having a structure capable of intercalating lithium ions, for example LiCoO 2 , LiMn 2 O 4 , LiNi 1 ⁇ x Co x O 2 (0 ⁇ x ⁇ 1).
- various carbon-based materials such as artificial graphite, natural graphite, and hard carbon, which intercalate and deintercalate lithium ions.
- the rechargeable lithium battery as its actuating power source has required much higher capacity.
- the rechargeable lithium battery in order to use the rechargeable lithium battery as an actuating power source or as a power storage source for a hybrid vehicle or an electric vehicle, research on development of a battery having satisfactory high rate capability, being rapidly charged and discharged, and having excellent cycle characteristics is actively made.
- Embodiments are directed to a positive active material for a rechargeable lithium battery including a core including a compound represented by Chemical Formula 1 and a structure-stabilizing compound on a surface of the core.
- the structure-stabilizing compound includes an Al compound or a Co compound
- Me is Mn or Al
- M 1 is Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, W, or a combination thereof.
- the structure-stabilizing compound may be Al 2 O 3 , Co 3 O 4 , Li a CoO 2 where a is 0.9 to 1.1, or a combination thereof.
- the structure-stabilizing compound may be a Co compound.
- the structure-stabilizing compound may be present as a layered phase or as an island shape on the surface of the core.
- a content of the structure-stabilizing compound may be about 1.5 wt % to about 3.0 wt % based on 100 wt % of the core.
- a surface of the positive active material may have a layered phase crystal structure.
- x may be in the range 0.8 ⁇ x ⁇ 0.9.
- Embodiments are also directed to a rechargeable lithium battery including a positive electrode including a positive active material as described above, a negative electrode including a negative active material, and an electrolyte.
- FIG. 1 illustrates a schematic view showing a structure of a positive active material according to an embodiment.
- FIG. 2 illustrates a graph showing discharge capacity results of half cells using the positive electrodes according to Experimental Examples 1 to 8.
- FIG. 3 illustrates a SEM image showing the positive active material according to Example 1.
- FIG. 4 illustrates TEM and SAD (selected area diffraction) images showing the positive active material according to Example 1.
- FIG. 5 illustrates a graph showing discharge capacity results of half cells using the positive electrodes according to Examples 1 to 3 and Reference Examples 1 to 3.
- FIG. 6 illustrates a graph showing room temperature cycle-life characteristic results of half cells using the positive electrodes according to Examples 1 to 3 and Reference Examples 1 to 3.
- a positive active material for a rechargeable lithium battery includes a core including a compound represented by Chemical Formula 1; and a structure-stabilizing compound disposed on a surface of the core and including an Al compound or a Co compound.
- Me is Mn or Al
- M 1 is Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, W, or a combination thereof.
- the positive active material has a high nickel content, with x being 0.7 to 0.93.
- x may be in the range, 0.8 ⁇ x ⁇ 0.9.
- Such a compound of Chemical Formula 1 having a high nickel content may be a compound having high capacity.
- the compound of Chemical Formula 1 where x is 0.7 to 0.93 may have a very high capacity compared with a compound having a low nickel content, for example, a compound where x is less than 0.7.
- M 1 is a doping element that substitutes some of a main element, Ni, Co, and Me constituting the positive active material of Chemical Formula 1.
- M 1 may be Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, or W.
- F is fluorine, as a doping element that substitutes a some of oxygen in the positive active material of Chemical Formula 1
- the structure-stabilizing compound may be Al 2 O 3 , Co 3 O 4 , Li a CoO 2 (where a is 0.9 to 1.1), or a combination thereof.
- the structure-stabilizing compound maybe in a form of a layered structure on the surface of the positive active material. Such a structure-stabilizing compound may improve mobility of lithium ions and in addition, may stabilize the structure of the core and thus improve initial efficiency and cycle-life characteristics of the positive active material.
- a compound core having a high nickel content that is, a compound core having x ranging from about 0.7 to about 0.93, includes unstable Ni in a higher amount than a compound core having x of less than 0.6 on the surface, an effect provided by the structure-stabilizing compound may be more effectively obtained.
- Li a CoO 2 may be formed through a reaction of a Co-containing precursor with Li included on the core and even inside the core when the Co-containing precursor is diffused into the core in the secondary heat-treating process during a process of manufacturing the positive active material.
- the Li a CoO 2 may be present on the surface of and/or inside the core.
- Li a CoO 2 When the Li a CoO 2 is included as a structure-stabilizing compound, a surface layered structure may be well developed, and thus, charge and discharge efficiency and a cycle-life may be improved.
- the structure-stabilizing compound may be a Co compound, for example, Co 3 O 4 , Li a CoO 2 , or a mixture of the Co 3 O 4 and the Li a CoO 2 .
- the structure-stabilizing compound is the mixture of the Co 3 O 4 and Li a CoO 2
- their mixing ratio may be in a range of greater than about 0 wt %: less than about 100 wt % to about 50:50.
- the mixing ratio of the Co 3 O 4 and the Li a CoO 2 is within the range, a coating process using the Co-containing precursor may be more effectively performed.
- the structure-stabilizing compound is a Co compound
- Co is more increasingly concentrated on the surface of the positive active material than in the core thereof, and resultantly, Ni may be less concentrated on the surface and may stabilize the surface structure.
- Ni when lithium ions are released from the core including a compound represented by Chemical Formula 1 during the charge and discharge, Ni may be oxidized into unstable tetravalent nickel and then, reduced to divalent nickel and thus may form NiO.
- the Co compound may suppress formation of the NiO and decrease resistance.
- the structure-stabilizing compound may be present as a layered phase (a continuous layer type) or an island shape (an non-continuous island type), or as both the layered phase and the island shape on the surface of the core.
- the structure-stabilizing compound may be more uniformly present and may provide a greater effect.
- the structure-stabilizing compound may be present on the surface of the core, and thus may reinforce the layer structure of the active material surface.
- the positive active material may have a layered phase crystal structure on the surface.
- the structure-stabilizing compound is present as a layered phase
- the active material surface may entirely have a layered phase crystal structure.
- the structure-stabilizing compound is present as an island shape
- the positive active material may have both a layered phase crystal structure and a mixed phase crystal structure.
- both a layered phase crystal structure and a mixed phase crystal structure may be obtained.
- a content of the structure-stabilizing compound may be about 1.5 wt % to about 3.0 wt %, or, for example, about 2.0 wt % to about 3.0 wt % based on 100 wt % of the core.
- excellent discharge capacity and cycle-life characteristics for example, room temperature cycle-life characteristics may be obtained.
- the positive active material according to an embodiment may be prepared by the following process.
- a lithium-containing compound, a nickel-containing compound, a cobalt-containing compound, and an Me-containing compound may be mixed. Additionally, an M 1 -containing compound or a fluorine-containing compound may be mixed to prepare a mixture.
- the lithium-containing compound may be a lithium acetate, a lithium nitrate, a lithium hydroxide, a lithium carbonate, a lithium acetate, a hydrate thereof, or a combination thereof.
- the nickel-containing compound may be a nickel nitrate, a nickel hydroxide, a nickel carbonate, a nickel acetate, a nickel sulfate, a hydrate thereof, or a combination thereof.
- the cobalt-containing compound may be a cobalt nitrate, a cobalt hydroxide, a cobalt acetate, a cobalt carbonate, a cobalt sulfate, a hydrate thereof, or a combination thereof and the Me-containing compound may be an Me-containing nitrate, an Me-containing hydroxide, an Me-containing carbonate, an Me-containing acetate, an Me-containing sulfate, a hydrate thereof, or a combination thereof.
- the NV-containing compound may be an NV-containing nitrate, an NV-containing hydroxide, an NV-containing carbonate, an NV-containing acetate, NV-containing oxide, an NV-containing sulfate
- the fluorine-containing compound may be a fluorine-containing nitrate, a fluorine-containing hydroxide, a fluorine-containing carbonate, a fluorine-containing acetate, a fluorine-containing sulfate, a fluorine-containing oxide, a hydrate thereof, or a combination thereof.
- a mixing ratio of the lithium-containing compound, the nickel-containing compound, the cobalt-containing compound, the Me-containing compound, the NV-containing compound, and the fluorine-containing compound may appropriately be controlled such that the compound of Chemical Formula 1 may be obtained.
- the mixture may be subject to a primary heat-treatment to prepare a core.
- the primary heat-treating process may be performed at about 700° C. to about 1000° C., for about 3 hours to about 20 hours.
- the primary heat-treating process may be performed under an oxygen O 2 atmosphere, or air atmosphere.
- the surface of the core may be coated with a precursor of a structure-stabilizing compound.
- the precursor of a structure-stabilizing compound may be Al(OH) 3 , Co(OH) 3 , Al 2 O 3 , Co 3 O 4 , or a combination thereof.
- the coating process may be performed in a wet process using a solvent or in a dry process without solvent.
- the solvent for the wet process may include water, ethyl alcohol, or isopropyl alcohol.
- the precursor of a structure-stabilizing compound may be mixed in an amount of about 1.5 wt % to about 3.0 wt % based on 100 wt % of the core.
- a secondary heat-treating process may be performed to prepare a positive active material.
- the secondary heat-treating process may be performed at about 500° C. to about 800° C. for about 5 hours to about 20 hours.
- a compound for forming the structure-stabilizing compound may be well diffused onto the surface of the core and may well form the structure-stabilizing compound on the surface of the core.
- Al(OH) 3 When Al(OH) 3 is used as a precursor of a structure-stabilizing compound, an Al 2 O 3 structure-stabilizing compound may be formed according to the secondary heat-treating process.
- Co(OH) 3 When Co(OH) 3 is used as a precursor of a structure-stabilizing compound, a part of Co(OH) may be diffused inside the core according to the secondary heat-treating process, and may react with Li included in the core such that Li a CoO 2 may be formed inside the core.
- Another embodiment provides a rechargeable lithium battery including the positive electrode including a positive active material, a negative electrode including a negative active material, and an electrolyte.
- the positive electrode may include a positive active material layer and a current collector supporting the positive active material.
- a content of the positive active material may be about 90 wt % to about 98 wt % based on the total amount of the positive active material layer.
- the positive active material layer may further include a binder and a conductive material.
- the binder and the conductive material may each be included in an amount of about 1 wt % to about 5 wt %, respectively, based on the total amount of the positive active material layer.
- the binder improves binding properties of positive active material particles with one another and with a current collector.
- the binder may include polyvinyl alcohol, carboxymethyl cellulose, hydroxypropyl cellulose, diacetyl cellulose, polyvinylchloride, carboxylated polyvinylchloride, polyvinylfluoride, an ethylene oxide-containing polymer, polyvinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, a styrene-butadiene rubber, an acrylated styrene-butadiene rubber, an epoxy resin, nylon, or the like.
- the conductive material is included to provide electrode conductivity.
- a suitable electrically conductive material that does not cause a chemical change may be used as a conductive material.
- the conductive material may be a carbon-based material such as natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, a carbon fiber, or the like; a metal-based material in a form of a metal powder or a metal fiber and including copper, nickel, aluminum, silver, or the like; a conductive polymer such as a polyphenylene derivative; or a mixture thereof.
- the current collector may be Al, as an example.
- the negative electrode may include a current collector and a negative active material layer formed on the current collector.
- the negative active material layer may include a negative active material.
- the negative active material includes a material that reversibly intercalates/deintercalates lithium ions, a lithium metal, a lithium metal alloy, a material being capable of doping/dedoping lithium, or a transition metal oxide.
- the material that can reversibly intercalate/deintercalate lithium ions may include a carbon material.
- the carbon material may be any generally-used carbon-based negative active material in a lithium ion rechargeable battery.
- Examples of the carbon material include crystalline carbon, amorphous carbon, and mixtures thereof.
- the crystalline carbon may be non-shaped, or sheet, flake, spherical, or fiber shaped natural graphite or artificial graphite.
- the amorphous carbon may be a soft carbon, a hard carbon, a mesophase pitch carbonization product, fired coke, or the like.
- lithium metal alloy examples include lithium and an element selected from Na, K, Rb, Cs, Fr, Be, Mg, Ca, Sr, Si, Sb, Pb, In, Zn, Ba, Ra, Ge, Al, and Sn.
- the material being capable of doping/dedoping lithium may include Si, a Si—C composite, SiO x (0 ⁇ x ⁇ 2), a Si-Q alloy (wherein Q is an element selected from an alkali metal, an alkaline-earth metal, a Group 13 element, a Group 14 element, a Group 15 element, a Group 16 element, a transition element, a rare earth element, and a combination thereof, and is not Si), Sn, SnO 2 , a Sn—R alloy (wherein R is an element selected from an alkali metal, an alkaline-earth metal, a Group 13 element, a Group 14 element, a Group 15 element, a Group 16 element, a transition element, a rare earth element, and a combination thereof, and is not Sn), or the like.
- Q is an element selected from an alkali metal, an alkaline-earth metal, a Group 13 element, a Group 14 element, a Group 15 element, a Group 16 element, a transition element,
- the elements Q and R may be selected from Mg, Ca, Sr, Ba, Ra, Sc, Y, Ti, Zr, Hf, Rf, V, Nb, Ta, Db, Cr, Mo, W, Sg, Tc, Re, Bh, Fe, Pb, Ru, Os, Hs, Rh, Ir, Pd, Pt, Cu, Ag, Au, Zn, Cd, B, Al, Ga, Sn, In, Tl, Ge, P, As, Sb, Bi, S, Se, Te, Po, and a combination thereof.
- the transition metal oxide may include vanadium oxide, lithium vanadium oxide, or the like.
- the negative active material may be included in an amount of about 95 wt % to about 99 wt % based on the total weight of the negative active material layer.
- the negative active material layer includes a binder, and optionally, a conductive material.
- the negative active material layer may include about 1 wt % to about 5 wt % of a binder based on the total weight of the negative active material layer.
- the negative active material layer may include about 90 wt % to about 98 wt % of the negative active material, about 1 wt % to about 5 wt % of the binder, and about 1 wt % to about 5 wt % of the conductive material.
- the binder improves binding properties of negative active material particles with one another and with a current collector.
- the binder may include a non-water-soluble binder, a water-soluble binder, or a combination thereof.
- the non-water-soluble binder includes polyvinylchloride, carboxylated polyvinylchloride, polyvinylfluoride, an ethylene oxide-containing polymer, polyvinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, polyamideimide, polyimide, or a combination thereof.
- the water-soluble binder may be a rubber-based binder or a polymer resin binder.
- the rubber-based binder may be selected from a styrene-butadiene rubber, an acrylated styrene-butadiene rubber (SBR), an acrylonitrile-butadiene rubber, an acrylic rubber, a butyl rubber, a fluorine rubber, and a combination thereof.
- the polymer resin binder may be selected from an ethylenepropylene copolymer, polyepichlorohydrine, polyphosphazene, polyacrylonitrile, polystyrene, an ethylenepropylenediene copolymer, polyvinylpyridine, chlorosulfonatedpolyethylene, a latex, a polyester resin, an acrylic resin, phenolic resin, an epoxy resin, polyvinyl alcohol, and a combination thereof.
- a cellulose-based compound may be further used as a thickener in order to provide viscosity.
- the cellulose-based compound includes one or more of carboxymethyl cellulose, hydroxypropylmethyl cellulose, methyl cellulose, or alkali metal salts thereof.
- the alkali metal may be Na, K, or Li.
- Such a thickener may be included in an amount of about 0.1 parts by weight to about 3 parts by weight based on 100 parts by weight of the negative active material.
- the conductive material may be included to provide electrode conductivity. Any suitable electrically conductive material that does not cause chemical chance may be used as a conductive material.
- the conductive material include a carbon-based material such as natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, a carbon fiber, or the like; a metal-based material of a metal powder or a metal fiber including copper, nickel, aluminum, silver, or the like; a conductive polymer such as a polyphenylene derivative; or a mixture thereof.
- the current collector may include one selected from a copper foil, a nickel foil, a stainless steel foil, a titanium foil, a nickel foam, a copper foam, a polymer substrate coated with a conductive metal, and a combination thereof, as examples.
- the electrolyte may include a non-aqueous organic solvent and a lithium salt.
- the non-aqueous organic solvent may serve as a medium for transmitting ions taking part in the electrochemical reaction of a battery.
- the non-aqueous organic solvent may include a carbonate-based, ester-based, ether-based, ketone-based, alcohol-based, or aprotic solvent.
- the carbonate based solvent may include dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropyl carbonate (EPC), methylethyl carbonate (MEC), ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), or the like.
- the ester-based solvent may include methyl acetate, ethyl acetate, n-propyl acetate, dimethylacetate, methylpropionate, ethylpropionate, ⁇ -butyrolactone, decanolide, valerolactone, mevalonolactone, caprolactone, or the like.
- the ether-based solvent include dibutyl ether, tetraglyme, diglyme, dimethoxyethane, 2-methyltetrahydrofuran, tetrahydrofuran, or the like.
- the ketone-based solvent includes cyclohexanone or the like.
- the alcohol-based solvent include ethyl alcohol, isopropyl alcohol, or the like.
- aprotic solvent examples include nitriles such as R—CN (where R is a C2 to C20 linear, branched, or cyclic hydrocarbon, a double bond, an aromatic ring, or an ether bond), amides such as dimethylformamide, dioxolanes such as 1,3-dioxolane, sulfolanes, and the like.
- the organic solvent may be used singularly or in a mixture.
- the mixture ratio may be controlled in accordance with a desirable battery performance.
- the carbonate-based solvent may include a mixture with a cyclic carbonate and a linear carbonate.
- the cyclic carbonate and linear carbonate may be mixed together in a volume ratio of about 1:1 to about 1:9.
- the electrolyte may have enhanced performance.
- the organic solvent may further include an aromatic hydrocarbon-based solvent as well as the carbonate-based solvent.
- the carbonate-based solvent and aromatic hydrocarbon-based solvent may be mixed together in a volume ratio of about 1:1 to about 30:1.
- the aromatic hydrocarbon-based organic solvent may be an aromatic hydrocarbon-based compound represented by Chemical Formula 2.
- R 1 to R 6 are the same or different and are selected from hydrogen, a halogen, a C1 to C10 alkyl group, a haloalkyl group, and a combination thereof.
- aromatic hydrocarbon-based organic solvent may be selected from benzene, fluorobenzene, 1,2-difluorobenzene, 1,3-difluorobenzene, 1,4-difluorobenzene, 1,2,3-trifluorobenzene, 1,2,4-trifluorobenzene, chlorobenzene, 1,2-dichlorobenzene, 1,3-dichlorobenzene, 1,4-dichlorobenzene, 1,2,3-trichlorobenzene, 1,2,4-trichlorobenzene, iodobenzene, 1,2-diiodobenzene, 1,3-diiodobenzene, 1,4-diiodobenzene, 1,2,3-triiodobenzene, 1,2,4-triiodobenzene, toluene, fluorotoluene, 2,3-difluorotoluene, 2,4-di
- the electrolyte may further include an additive of vinylene carbonate, an ethylene carbonate-based compound represented by Chemical Formula 3, or propanesultone to improve cycle life.
- R 7 and R 8 are the same or different and may be each independently hydrogen, a halogen, a cyano group (CN), a nitro group (NO 2 ), or a C1 to C5 fluoroalkyl group, provided that at least one of R 7 and R 8 is a halogen, a cyano group (CN), a nitro group (NO 2 ), or a C1 to C5 fluoroalkyl group, and R 7 and R 8 are not simultaneously hydrogen.
- Examples of the ethylene carbonate-based compound include difluoroethylene carbonate, chloroethylene carbonate, dichloroethylene carbonate, bromoethylene carbonate, dibromoethylene carbonate, nitroethylene carbonate, cyanoethylene carbonate, vinylethylene carbonate, fluoroethylene carbonate, or the like.
- the amount of the additive for improving cycle life may be flexibly used within an appropriate range.
- the lithium salt dissolved in an organic solvent supplies a battery with lithium ions, basically operates the rechargeable lithium battery, and improves transportation of the lithium ions between positive and negative electrodes.
- the lithium salt include at least one supporting salt selected from LiPF 6 , LiBF 4 , LiSbF 6 , LiAsF 6 , LiN(SO 2 C 2 F 5 ) 2 , Li(CF 3 SO 2 ) 2 N, LiN(SO 3 C 2 F 5 ) 2 , LiC 4 F 9 SO 3 , LiClO 4 , LiAlO 2 , LiAlCl 4 , LiN(C x F 2x+1 SO 2 )(C y F 2y+1 SO 2 ) (where x and y are natural numbers, for example, integers of 1 to 20), LiCl, LiI, and LiB(C 2 O 4 ) 2 (lithium bis(oxalato) borate; LiBOB).
- the lithium salt may be used in a concentration ranging from about 0.1 M to about 2.0 M.
- an electrolyte may have excellent performance and lithium ion mobility due to optimal electrolyte conductivity and viscosity.
- the rechargeable lithium battery may further include a separator between the negative electrode and the positive electrode, depending on a kind of the battery.
- a suitable separator material include polyethylene, polypropylene, polyvinylidene fluoride, and multi-layers thereof such as a polyethylene/polypropylene double-layered separator, a polyethylene/polypropylene/polyethylene triple-layered separator, and a polypropylene/polyethylene/polypropylene triple-layered separator.
- FIG. 1 illustrates an exploded partial perspective view of a rechargeable lithium battery according to an embodiment.
- the rechargeable lithium battery may one of variously-shaped batteries such as a cylindrical battery, a pouch battery, or the like.
- the rechargeable lithium battery may be a prismatic rechargeable lithium battery.
- a rechargeable lithium battery 100 may include an electrode assembly 40 manufactured by winding a separator 30 interposed between a positive electrode 10 and a negative electrode 20 , and a case 50 housing the electrode assembly 40 .
- An electrolyte may be impregnated in the positive electrode 10 , the negative electrode 20 , and the separator 30 .
- the case may be sealed, for example, by a cover or cap or other form of sealing member, depending on the type of rechargeable lithium battery.
- Electrode tabs or terminals electrically connected to the positive electrode 10 and the negative electrode 20 may be outside the case.
- the mixture was heat-treated at 740° C. under an oxygen (O 2 ) atmosphere for 20 hours to prepare a LiNi 0.5 Co 0.2 Mn 0.3 O 2 positive active material.
- a positive active material composition 94 wt % of the prepared positive active material, 3 wt % of a polyvinylidene fluoride binder, and 3 wt % of a ketjen black conductive material were mixed or dissolved in an N-methylpyrrolidone solvent to prepare a positive active material composition.
- the positive active material composition was coated onto an Al current collector to manufacture a positive electrode.
- the positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- the positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- the positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- the positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- the positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- the positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- the positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- Each positive electrode according to Experimental Examples 1 to 8, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method.
- the electrolyte was prepared by dissolving 1.0 M LiPF 6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- the half-cell was charged and discharged at 25° C. within a range of 3.0 V to 4.3 V at 0.2 C. Then, the discharge capacity of the half-cell was measured.
- the results for Experimental Examples 1 to 8 are provided in FIG. 2 . (The circles in FIG. 2 correspond to Experimental Examples 1 to 8 in order, from left to right.)
- the mixture was primarily heat-treated at 740° C. under an oxygen (O 2 ) atmosphere for 20 hours to prepare a LiNi 0.85 Co 0.135 Al 0.015 O 2 core.
- the Co 3 O 4 and Li a CoO 2 structure-stabilizing compound was present as an island shape and a layered phase on the surface of the core.
- the structure-stabilizing compound was present in an amount of 1.5 wt % based on 100 wt % of the core in the final positive active material.
- 94 wt % of the prepared positive active material, 3 wt % of a polyvinylidene fluoride binder, and 3 wt % of a ketjen black conductive material were mixed or dissolved in an N-methylpyrrolidone solvent to prepare a positive active material composition.
- the positive active material composition was coated onto an Al current collector to manufacture a positive electrode.
- the structure-stabilizing compound was present in an amount of 2 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 3 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 0.5 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 1 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 5 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- FIG. 3 illustrates a SEM image showing the positive active material of Example 1.
- the positive active material of Example 1 has a Co-including structure-stabilizing compound coated as an island shape and a layered phase on the surface of the core.
- FIG. 4( a ) illustrates a TEM image showing the positive active material of Example 1
- FIG. 4( b ) illustrates a SAD (selected area diffraction) image showing the surface corresponding to area 1 in FIG. 4( a )
- FIG. 4 c ) of FIG. 4 illustrates a SAD (selected area diffraction) image showing the surface corresponding to area 2 in ( FIG. 4 a ).
- the surface of the positive active material of Example 1 had a layered crystal structure and a mixed crystal structure.
- Each positive electrode according to Examples 1 to 3 and Reference Examples 1 to 3, a lithium metal counter electrode, and an electrolyte were used to manufacture in a coin-type half-cell in a general method.
- the electrolyte was prepared by dissolving 1.3 M LiPF 6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- the manufactured half-cell was charged and discharged 50 times at 25° C. in a range of 3.0 V to 4.3 V at 0.2 C, and discharge capacity of the half-cell was measured. In addition, a capacity retention was obtained by calculating a ratio of the 50th discharge capacity relative to the first discharge capacity as a cycle-life.
- the half-cells respectively using the positive electrodes using a positive active material including Co 3 O 4 and Li a CoO 2 as a structure-stabilizing compound in a range of 1.5 wt % to 3 wt % according to Examples 1 to 3 exhibited discharge capacity of greater than or equal to 200 mAh/g and cycle-life characteristics of greater than or equal to 85%.
- the half-cells including the structure-stabilizing compound in a smaller amount than the range according to Reference Examples 1 and 2 and the half-cells including the structure-stabilizing compound in a larger amount than the range according to Reference Example 3 exhibited deteriorated capacity and cycle-life characteristics.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- Each positive electrode according to Example 1 and Comparative Example 1, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method.
- the electrolyte was prepared by dissolving 1.3 M LiPF 6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- the half-cells were charged and discharged once at 0.1 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm 2 to perform a formation process.
- the charge and discharge capacities and efficiencies of the half-cells were measured, and the results are shown in Table 2.
- the cells were charged and discharged once at 0.2 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm 2 .
- the discharge capacities of the half cells were measured, and the results are shown in Table 2.
- the positive active material having a structure-stabilizing compound on the surface according to Example 1 exhibited excellent charge and discharge characteristics compared with the positive active material including no structure-stabilizing compound according to Comparative Example 1.
- the mixture was subjected to a primary heat-treatment at 740° C. under an oxygen (O 2 ) atmosphere for 20 hours to prepare a LiNi 0.85 Co 0.135 Mn 0.015 O 2 core.
- the Co 3 O 4 and Li a CoO 2 structure-stabilizing compound was present as an island shape and a layered phase on the surface of the core.
- the structure-stabilizing compound was included in an amount of 1.5 wt % based on 100 wt % of the core.
- a positive active material composition 94 wt % of the prepared positive active material, 3 wt % of a polyvinylidene fluoride binder, and 3 wt % of a ketjen black conductive material were mixed or dissolved in an N-methylpyrrolidone solvent to prepare a positive active material composition.
- the positive active material composition was coated onto an Al current collector to manufacture a positive electrode.
- the structure-stabilizing compound was present in an amount of 2 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 3 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 0.5 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 1 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- the structure-stabilizing compound was present in an amount of 5 wt % based on 100 wt % of the core.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- Each positive electrode according to Examples 4 to 6 and Reference Examples 4 to 6, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method.
- the electrolyte was prepared by dissolving 1.3 M LiPF 6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 of a volume ratio).
- the manufactured half-cells were charged and discharged 50 times at 25° C. in a range of 3.0 V to 4.3 Vat 0.2 C, and the discharge capacities of the half-cells were measured.
- a capacity retention value was obtained by calculating a ratio of the 50th discharge capacity relative to the first discharge capacity to evaluate a cycle-life.
- the half-cells using the positive electrodes using the positive active material including Co 3 O 4 and Li a CoO 2 in an amount of 1.5 wt % to 3 wt % as a structure-stabilizing compound according to Examples 4 to 6 showed discharge capacity of greater than or equal to 200 mAh/g and cycle-life characteristics of greater than or equal to 85%, while the half-cells including the structure-stabilizing compound in a smaller amount than the range according to Reference Examples 4 and 5 and the half-cells including the structure-stabilizing compound in a larger amount than the range according to Reference Example 6 exhibited deteriorated cycle-life characteristics.
- a positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- Each positive electrode according to Example 4 and Comparative Example 2, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method.
- the electrolyte was prepared by dissolving 1.3 M LiPF 6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- the manufactured half-cells were charged and discharged once at 0.1 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm 2 to perform a formation process.
- the charge and discharge capacities and efficiencies of the half-cells were obtained, and the results are shown in Table 4.
- the cells were charged and discharged once at 0.2 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm 2 .
- the discharge capacities of the half-cells were obtained, and the results are shown in Table 4.
- the positive active material having the structure-stabilizing compound on the surface according to Example 4 showed excellent charge and discharge characteristics compared with the positive active material including no structure-stabilizing compound according to Comparative Example 2.
- a rechargeable lithium battery includes a positive electrode, a negative electrode, and an electrolyte.
- a positive active material of a positive electrode may be an oxide including lithium and a transition metal and having a structure capable of intercalating lithium ions.
- the positive active material may be LiCoO 2 , LiMn 2 O 4 , or LiNi 1 ⁇ x Co x O 2 (0 ⁇ x ⁇ 1).
- various carbon-based materials such as artificial graphite, natural graphite, and hard carbon, which intercalate and deintercalate lithium ions.
- Embodiments provide a positive active material for a rechargeable lithium battery having high capacity and excellent cycle-life characteristics.
- Embodiment provide a rechargeable lithium battery including the positive active material.
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Abstract
A positive active material for a rechargeable lithium battery includes a core including a compound represented by Chemical Formula 1 and a structure-stabilizing compound on a surface of the core. The structure-stabilizing compound includes an Al compound or a Co compound. Chemical Formula 1 is LiaNixCoyMezM1 kO2−pFp where 0.9≤a≤1.1, 0.7≤x≤0.93, 0<y≤0.3, 0<z≤0.3, 0≤k≤0.005, x+y+z+k=1, 0≤p≤0.005, Me is Mn or Al, and Ml is Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, W, or a combination thereof.
Description
- This is a divisional application based on pending application Ser. No. 15/487,635, filed Apr. 14, 2017, the entire contents of which is hereby incorporated by reference.
- Korean Patent Application No. 10-2016-0046345, filed on Apr. 15, 2016, in the Korean Intellectual Property Office, and entitled: “Positive Active Material for Rechargeable Lithium Battery and Rechargeable Lithium Battery Including Same,” is incorporated by reference herein in its entirety.
- Embodiments are directed to a positive active material for a rechargeable lithium battery and a rechargeable lithium battery including the same.
- A rechargeable lithium battery may be used as an actuating power source for a mobile information terminal such as a cell phone, a laptop, a smart phone, and the like.
- The rechargeable lithium battery includes a positive electrode, a negative electrode, and an electrolyte. Herein, for a positive active material of a positive electrode may be an oxide consisting of lithium and a transition metal and having a structure capable of intercalating lithium ions, for example LiCoO2, LiMn2O4, LiNi1−xCoxO2 (0<x<1).
- As for a negative active material, various carbon-based materials such as artificial graphite, natural graphite, and hard carbon, which intercalate and deintercalate lithium ions.
- Recently, as the mobile information terminal has been rapidly down-sized and lightened the rechargeable lithium battery as its actuating power source has required much higher capacity. In addition, in order to use the rechargeable lithium battery as an actuating power source or as a power storage source for a hybrid vehicle or an electric vehicle, research on development of a battery having satisfactory high rate capability, being rapidly charged and discharged, and having excellent cycle characteristics is actively made.
- Embodiments are directed to a positive active material for a rechargeable lithium battery including a core including a compound represented by Chemical Formula 1 and a structure-stabilizing compound on a surface of the core. The structure-stabilizing compound includes an Al compound or a Co compound
-
LiaNixCoyMezM1 kO2−pFp [Chemical Formula 1] - wherein, 0.9≤a≤1.1, 0.7≤x≤0.93, 0<y≤0.3, 0≤z≤0.3, 0≤k≤0.005, x+y+z+k=1, 0≤p≤0.005, Me is Mn or Al, and M1 is Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, W, or a combination thereof.
- The structure-stabilizing compound may be Al2O3, Co3O4, LiaCoO2 where a is 0.9 to 1.1, or a combination thereof.
- The structure-stabilizing compound may be a Co compound.
- The structure-stabilizing compound may be present as a layered phase or as an island shape on the surface of the core.
- A content of the structure-stabilizing compound may be about 1.5 wt % to about 3.0 wt % based on 100 wt % of the core.
- A surface of the positive active material may have a layered phase crystal structure.
- In Chemical Formula 1, x may be in the range 0.8≤x≤0.9.
- Embodiments are also directed to a rechargeable lithium battery including a positive electrode including a positive active material as described above, a negative electrode including a negative active material, and an electrolyte.
- Features will become apparent to those of skill in the art by describing in detail exemplary embodiments with reference to the attached drawings in which:
-
FIG. 1 illustrates a schematic view showing a structure of a positive active material according to an embodiment. -
FIG. 2 illustrates a graph showing discharge capacity results of half cells using the positive electrodes according to Experimental Examples 1 to 8. -
FIG. 3 illustrates a SEM image showing the positive active material according to Example 1. -
FIG. 4 illustrates TEM and SAD (selected area diffraction) images showing the positive active material according to Example 1. -
FIG. 5 illustrates a graph showing discharge capacity results of half cells using the positive electrodes according to Examples 1 to 3 and Reference Examples 1 to 3. -
FIG. 6 illustrates a graph showing room temperature cycle-life characteristic results of half cells using the positive electrodes according to Examples 1 to 3 and Reference Examples 1 to 3. - Example embodiments will now be described more fully hereinafter with reference to the accompanying drawings; however, they may be embodied in different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete, and will fully convey exemplary implementations to those skilled in the art.
- A positive active material for a rechargeable lithium battery according to an embodiment includes a core including a compound represented by
Chemical Formula 1; and a structure-stabilizing compound disposed on a surface of the core and including an Al compound or a Co compound. -
LiaNixCoyMezM1 kO2−pFp [Chemical Formula 1] - In
Chemical Formula 1, 0.9≤a≤1.1, 0.7≤x≤0.93, 0≤y≤0.3, 0<z≤0.3, 0≤k≤0.005, x+y+z+k=1, 0≤p≤0.005, - Me is Mn or Al, and
- M1 is Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, W, or a combination thereof.
- The positive active material has a high nickel content, with x being 0.7 to 0.93. For example, in
Chemical Formula 1, x may be in the range, 0.8≤x≤0.9. - Such a compound of
Chemical Formula 1 having a high nickel content, for example, with x being 0.7 to 0.93, may be a compound having high capacity. The compound ofChemical Formula 1 where x is 0.7 to 0.93 may have a very high capacity compared with a compound having a low nickel content, for example, a compound where x is less than 0.7. - In
Chemical Formula 1, M1 is a doping element that substitutes some of a main element, Ni, Co, and Me constituting the positive active material ofChemical Formula 1. Examples of M1 may be Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, or W. In addition, F is fluorine, as a doping element that substitutes a some of oxygen in the positive active material ofChemical Formula 1 - The structure-stabilizing compound may be Al2O3, Co3O4, LiaCoO2 (where a is 0.9 to 1.1), or a combination thereof. The structure-stabilizing compound maybe in a form of a layered structure on the surface of the positive active material. Such a structure-stabilizing compound may improve mobility of lithium ions and in addition, may stabilize the structure of the core and thus improve initial efficiency and cycle-life characteristics of the positive active material.
- In addition, when a compound core having a high nickel content, that is, a compound core having x ranging from about 0.7 to about 0.93, includes unstable Ni in a higher amount than a compound core having x of less than 0.6 on the surface, an effect provided by the structure-stabilizing compound may be more effectively obtained.
- Among the structure-stabilizing compounds, LiaCoO2 may be formed through a reaction of a Co-containing precursor with Li included on the core and even inside the core when the Co-containing precursor is diffused into the core in the secondary heat-treating process during a process of manufacturing the positive active material. For example, the LiaCoO2 may be present on the surface of and/or inside the core.
- When the LiaCoO2 is included as a structure-stabilizing compound, a surface layered structure may be well developed, and thus, charge and discharge efficiency and a cycle-life may be improved.
- In particular, the structure-stabilizing compound may be a Co compound, for example, Co3O4, LiaCoO2, or a mixture of the Co3O4 and the LiaCoO2. When the structure-stabilizing compound is the mixture of the Co3O4 and LiaCoO2, their mixing ratio may be in a range of greater than about 0 wt %: less than about 100 wt % to about 50:50. When the mixing ratio of the Co3O4 and the LiaCoO2 is within the range, a coating process using the Co-containing precursor may be more effectively performed. When the structure-stabilizing compound is a Co compound, Co is more increasingly concentrated on the surface of the positive active material than in the core thereof, and resultantly, Ni may be less concentrated on the surface and may stabilize the surface structure. In addition, when lithium ions are released from the core including a compound represented by
Chemical Formula 1 during the charge and discharge, Ni may be oxidized into unstable tetravalent nickel and then, reduced to divalent nickel and thus may form NiO. The Co compound may suppress formation of the NiO and decrease resistance. - The structure-stabilizing compound may be present as a layered phase (a continuous layer type) or an island shape (an non-continuous island type), or as both the layered phase and the island shape on the surface of the core. When the structure-stabilizing compound is present as the layered phase on the surface of the core, the structure-stabilizing compound may be more uniformly present and may provide a greater effect.
- The structure-stabilizing compound may be present on the surface of the core, and thus may reinforce the layer structure of the active material surface. For example, the positive active material may have a layered phase crystal structure on the surface. When the structure-stabilizing compound is present as a layered phase, the active material surface may entirely have a layered phase crystal structure. When the structure-stabilizing compound is present as an island shape, the positive active material may have both a layered phase crystal structure and a mixed phase crystal structure. When the structure-stabilizing compound is present as both layered phase and island shape, both a layered phase crystal structure and a mixed phase crystal structure may be obtained.
- A content of the structure-stabilizing compound may be about 1.5 wt % to about 3.0 wt %, or, for example, about 2.0 wt % to about 3.0 wt % based on 100 wt % of the core. When the structure-stabilizing compound is included within the ranges, excellent discharge capacity and cycle-life characteristics, for example, room temperature cycle-life characteristics may be obtained.
- The positive active material according to an embodiment may be prepared by the following process.
- A lithium-containing compound, a nickel-containing compound, a cobalt-containing compound, and an Me-containing compound may be mixed. Additionally, an M1-containing compound or a fluorine-containing compound may be mixed to prepare a mixture.
- The lithium-containing compound may be a lithium acetate, a lithium nitrate, a lithium hydroxide, a lithium carbonate, a lithium acetate, a hydrate thereof, or a combination thereof. The nickel-containing compound may be a nickel nitrate, a nickel hydroxide, a nickel carbonate, a nickel acetate, a nickel sulfate, a hydrate thereof, or a combination thereof. The cobalt-containing compound may be a cobalt nitrate, a cobalt hydroxide, a cobalt acetate, a cobalt carbonate, a cobalt sulfate, a hydrate thereof, or a combination thereof and the Me-containing compound may be an Me-containing nitrate, an Me-containing hydroxide, an Me-containing carbonate, an Me-containing acetate, an Me-containing sulfate, a hydrate thereof, or a combination thereof. The NV-containing compound may be an NV-containing nitrate, an NV-containing hydroxide, an NV-containing carbonate, an NV-containing acetate, NV-containing oxide, an NV-containing sulfate, and the fluorine-containing compound may be a fluorine-containing nitrate, a fluorine-containing hydroxide, a fluorine-containing carbonate, a fluorine-containing acetate, a fluorine-containing sulfate, a fluorine-containing oxide, a hydrate thereof, or a combination thereof.
- A mixing ratio of the lithium-containing compound, the nickel-containing compound, the cobalt-containing compound, the Me-containing compound, the NV-containing compound, and the fluorine-containing compound may appropriately be controlled such that the compound of
Chemical Formula 1 may be obtained. - The mixture may be subject to a primary heat-treatment to prepare a core. The primary heat-treating process may be performed at about 700° C. to about 1000° C., for about 3 hours to about 20 hours. The primary heat-treating process may be performed under an oxygen O2 atmosphere, or air atmosphere.
- The surface of the core may be coated with a precursor of a structure-stabilizing compound. The precursor of a structure-stabilizing compound may be Al(OH)3, Co(OH)3, Al2O3, Co3O4, or a combination thereof.
- The coating process may be performed in a wet process using a solvent or in a dry process without solvent. The solvent for the wet process may include water, ethyl alcohol, or isopropyl alcohol.
- In a process of coating a precursor of a structure-stabilizing compound on the surface of the core, the precursor of a structure-stabilizing compound may be mixed in an amount of about 1.5 wt % to about 3.0 wt % based on 100 wt % of the core.
- After the coating process, a secondary heat-treating process may be performed to prepare a positive active material. The secondary heat-treating process may be performed at about 500° C. to about 800° C. for about 5 hours to about 20 hours. When the secondary heat-treating process is performed within the temperature and time ranges, a compound for forming the structure-stabilizing compound may be well diffused onto the surface of the core and may well form the structure-stabilizing compound on the surface of the core.
- When Al(OH)3 is used as a precursor of a structure-stabilizing compound, an Al2O3 structure-stabilizing compound may be formed according to the secondary heat-treating process. When Co(OH)3 is used as a precursor of a structure-stabilizing compound, a part of Co(OH) may be diffused inside the core according to the secondary heat-treating process, and may react with Li included in the core such that LiaCoO2 may be formed inside the core.
- Another embodiment provides a rechargeable lithium battery including the positive electrode including a positive active material, a negative electrode including a negative active material, and an electrolyte.
- The positive electrode may include a positive active material layer and a current collector supporting the positive active material. In the positive active material layer, a content of the positive active material may be about 90 wt % to about 98 wt % based on the total amount of the positive active material layer.
- In an embodiment, the positive active material layer may further include a binder and a conductive material. The binder and the conductive material may each be included in an amount of about 1 wt % to about 5 wt %, respectively, based on the total amount of the positive active material layer.
- The binder improves binding properties of positive active material particles with one another and with a current collector. Examples of the binder may include polyvinyl alcohol, carboxymethyl cellulose, hydroxypropyl cellulose, diacetyl cellulose, polyvinylchloride, carboxylated polyvinylchloride, polyvinylfluoride, an ethylene oxide-containing polymer, polyvinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, a styrene-butadiene rubber, an acrylated styrene-butadiene rubber, an epoxy resin, nylon, or the like.
- The conductive material is included to provide electrode conductivity. A suitable electrically conductive material that does not cause a chemical change may be used as a conductive material. Examples of the conductive material may be a carbon-based material such as natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, a carbon fiber, or the like; a metal-based material in a form of a metal powder or a metal fiber and including copper, nickel, aluminum, silver, or the like; a conductive polymer such as a polyphenylene derivative; or a mixture thereof.
- The current collector may be Al, as an example.
- The negative electrode may include a current collector and a negative active material layer formed on the current collector. The negative active material layer may include a negative active material.
- The negative active material includes a material that reversibly intercalates/deintercalates lithium ions, a lithium metal, a lithium metal alloy, a material being capable of doping/dedoping lithium, or a transition metal oxide.
- The material that can reversibly intercalate/deintercalate lithium ions may include a carbon material. The carbon material may be any generally-used carbon-based negative active material in a lithium ion rechargeable battery. Examples of the carbon material include crystalline carbon, amorphous carbon, and mixtures thereof. The crystalline carbon may be non-shaped, or sheet, flake, spherical, or fiber shaped natural graphite or artificial graphite. The amorphous carbon may be a soft carbon, a hard carbon, a mesophase pitch carbonization product, fired coke, or the like.
- Examples of the lithium metal alloy include lithium and an element selected from Na, K, Rb, Cs, Fr, Be, Mg, Ca, Sr, Si, Sb, Pb, In, Zn, Ba, Ra, Ge, Al, and Sn.
- The material being capable of doping/dedoping lithium may include Si, a Si—C composite, SiOx (0<x<2), a Si-Q alloy (wherein Q is an element selected from an alkali metal, an alkaline-earth metal, a Group 13 element, a Group 14 element, a Group 15 element, a Group 16 element, a transition element, a rare earth element, and a combination thereof, and is not Si), Sn, SnO2, a Sn—R alloy (wherein R is an element selected from an alkali metal, an alkaline-earth metal, a Group 13 element, a Group 14 element, a Group 15 element, a Group 16 element, a transition element, a rare earth element, and a combination thereof, and is not Sn), or the like. At least one of these materials may be mixed with SiO2. The elements Q and R may be selected from Mg, Ca, Sr, Ba, Ra, Sc, Y, Ti, Zr, Hf, Rf, V, Nb, Ta, Db, Cr, Mo, W, Sg, Tc, Re, Bh, Fe, Pb, Ru, Os, Hs, Rh, Ir, Pd, Pt, Cu, Ag, Au, Zn, Cd, B, Al, Ga, Sn, In, Tl, Ge, P, As, Sb, Bi, S, Se, Te, Po, and a combination thereof.
- The transition metal oxide may include vanadium oxide, lithium vanadium oxide, or the like.
- In the negative active material layer, the negative active material may be included in an amount of about 95 wt % to about 99 wt % based on the total weight of the negative active material layer.
- In an embodiment, the negative active material layer includes a binder, and optionally, a conductive material. The negative active material layer may include about 1 wt % to about 5 wt % of a binder based on the total weight of the negative active material layer. When the negative active material layer includes a conductive material, the negative active material layer may include about 90 wt % to about 98 wt % of the negative active material, about 1 wt % to about 5 wt % of the binder, and about 1 wt % to about 5 wt % of the conductive material.
- The binder improves binding properties of negative active material particles with one another and with a current collector. The binder may include a non-water-soluble binder, a water-soluble binder, or a combination thereof.
- The non-water-soluble binder includes polyvinylchloride, carboxylated polyvinylchloride, polyvinylfluoride, an ethylene oxide-containing polymer, polyvinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, polyamideimide, polyimide, or a combination thereof.
- The water-soluble binder may be a rubber-based binder or a polymer resin binder. The rubber-based binder may be selected from a styrene-butadiene rubber, an acrylated styrene-butadiene rubber (SBR), an acrylonitrile-butadiene rubber, an acrylic rubber, a butyl rubber, a fluorine rubber, and a combination thereof. The polymer resin binder may be selected from an ethylenepropylene copolymer, polyepichlorohydrine, polyphosphazene, polyacrylonitrile, polystyrene, an ethylenepropylenediene copolymer, polyvinylpyridine, chlorosulfonatedpolyethylene, a latex, a polyester resin, an acrylic resin, phenolic resin, an epoxy resin, polyvinyl alcohol, and a combination thereof.
- When the water-soluble binder is used as a negative electrode binder, a cellulose-based compound may be further used as a thickener in order to provide viscosity. The cellulose-based compound includes one or more of carboxymethyl cellulose, hydroxypropylmethyl cellulose, methyl cellulose, or alkali metal salts thereof. The alkali metal may be Na, K, or Li. Such a thickener may be included in an amount of about 0.1 parts by weight to about 3 parts by weight based on 100 parts by weight of the negative active material.
- The conductive material may be included to provide electrode conductivity. Any suitable electrically conductive material that does not cause chemical chance may be used as a conductive material. Examples of the conductive material include a carbon-based material such as natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, a carbon fiber, or the like; a metal-based material of a metal powder or a metal fiber including copper, nickel, aluminum, silver, or the like; a conductive polymer such as a polyphenylene derivative; or a mixture thereof.
- The current collector may include one selected from a copper foil, a nickel foil, a stainless steel foil, a titanium foil, a nickel foam, a copper foam, a polymer substrate coated with a conductive metal, and a combination thereof, as examples.
- The electrolyte may include a non-aqueous organic solvent and a lithium salt.
- The non-aqueous organic solvent may serve as a medium for transmitting ions taking part in the electrochemical reaction of a battery.
- The non-aqueous organic solvent may include a carbonate-based, ester-based, ether-based, ketone-based, alcohol-based, or aprotic solvent.
- The carbonate based solvent may include dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropyl carbonate (EPC), methylethyl carbonate (MEC), ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), or the like. The ester-based solvent may include methyl acetate, ethyl acetate, n-propyl acetate, dimethylacetate, methylpropionate, ethylpropionate, γ-butyrolactone, decanolide, valerolactone, mevalonolactone, caprolactone, or the like. The ether-based solvent include dibutyl ether, tetraglyme, diglyme, dimethoxyethane, 2-methyltetrahydrofuran, tetrahydrofuran, or the like. The ketone-based solvent includes cyclohexanone or the like. The alcohol-based solvent include ethyl alcohol, isopropyl alcohol, or the like. Examples of the aprotic solvent include nitriles such as R—CN (where R is a C2 to C20 linear, branched, or cyclic hydrocarbon, a double bond, an aromatic ring, or an ether bond), amides such as dimethylformamide, dioxolanes such as 1,3-dioxolane, sulfolanes, and the like.
- The organic solvent may be used singularly or in a mixture. When the organic solvent is used in a mixture, the mixture ratio may be controlled in accordance with a desirable battery performance.
- The carbonate-based solvent may include a mixture with a cyclic carbonate and a linear carbonate. The cyclic carbonate and linear carbonate may be mixed together in a volume ratio of about 1:1 to about 1:9. When the mixture is used as an electrolyte, the electrolyte may have enhanced performance.
- The organic solvent may further include an aromatic hydrocarbon-based solvent as well as the carbonate-based solvent. The carbonate-based solvent and aromatic hydrocarbon-based solvent may be mixed together in a volume ratio of about 1:1 to about 30:1.
- The aromatic hydrocarbon-based organic solvent may be an aromatic hydrocarbon-based compound represented by
Chemical Formula 2. - In
Chemical Formula 2, R1 to R6 are the same or different and are selected from hydrogen, a halogen, a C1 to C10 alkyl group, a haloalkyl group, and a combination thereof. - Specific examples of the aromatic hydrocarbon-based organic solvent may be selected from benzene, fluorobenzene, 1,2-difluorobenzene, 1,3-difluorobenzene, 1,4-difluorobenzene, 1,2,3-trifluorobenzene, 1,2,4-trifluorobenzene, chlorobenzene, 1,2-dichlorobenzene, 1,3-dichlorobenzene, 1,4-dichlorobenzene, 1,2,3-trichlorobenzene, 1,2,4-trichlorobenzene, iodobenzene, 1,2-diiodobenzene, 1,3-diiodobenzene, 1,4-diiodobenzene, 1,2,3-triiodobenzene, 1,2,4-triiodobenzene, toluene, fluorotoluene, 2,3-difluorotoluene, 2,4-difluorotoluene, 2,5-difluorotoluene, 2,3,4-trifluorotoluene, 2,3,5-trifluorotoluene, chlorotoluene, 2,3-dichlorotoluene, 2,4-dichlorotoluene, 2,5-dichlorotoluene, 2,3,4-trichlorotoluene, 2,3,5-trichlorotoluene, iodotoluene, 2,3-diiodotoluene, 2,4-diiodotoluene, 2,5-diiodotoluene, 2,3,4-triiodotoluene, 2,3,5-triiodotoluene, xylene, and a combination thereof.
- The electrolyte may further include an additive of vinylene carbonate, an ethylene carbonate-based compound represented by
Chemical Formula 3, or propanesultone to improve cycle life. - In
Chemical Formula 3, R7 and R8 are the same or different and may be each independently hydrogen, a halogen, a cyano group (CN), a nitro group (NO2), or a C1 to C5 fluoroalkyl group, provided that at least one of R7 and R8 is a halogen, a cyano group (CN), a nitro group (NO2), or a C1 to C5 fluoroalkyl group, and R7 and R8 are not simultaneously hydrogen. - Examples of the ethylene carbonate-based compound include difluoroethylene carbonate, chloroethylene carbonate, dichloroethylene carbonate, bromoethylene carbonate, dibromoethylene carbonate, nitroethylene carbonate, cyanoethylene carbonate, vinylethylene carbonate, fluoroethylene carbonate, or the like. The amount of the additive for improving cycle life may be flexibly used within an appropriate range.
- The lithium salt dissolved in an organic solvent supplies a battery with lithium ions, basically operates the rechargeable lithium battery, and improves transportation of the lithium ions between positive and negative electrodes. Examples of the lithium salt include at least one supporting salt selected from LiPF6, LiBF4, LiSbF6, LiAsF6, LiN(SO2C2F5)2, Li(CF3SO2)2N, LiN(SO3C2F5)2, LiC4F9SO3, LiClO4, LiAlO2, LiAlCl4, LiN(CxF2x+1SO2)(CyF2y+1SO2) (where x and y are natural numbers, for example, integers of 1 to 20), LiCl, LiI, and LiB(C2O4)2 (lithium bis(oxalato) borate; LiBOB). The lithium salt may be used in a concentration ranging from about 0.1 M to about 2.0 M. When the lithium salt is included at the above concentration range, an electrolyte may have excellent performance and lithium ion mobility due to optimal electrolyte conductivity and viscosity.
- The rechargeable lithium battery may further include a separator between the negative electrode and the positive electrode, depending on a kind of the battery. Examples of a suitable separator material include polyethylene, polypropylene, polyvinylidene fluoride, and multi-layers thereof such as a polyethylene/polypropylene double-layered separator, a polyethylene/polypropylene/polyethylene triple-layered separator, and a polypropylene/polyethylene/polypropylene triple-layered separator.
-
FIG. 1 illustrates an exploded partial perspective view of a rechargeable lithium battery according to an embodiment. The rechargeable lithium battery may one of variously-shaped batteries such as a cylindrical battery, a pouch battery, or the like. For example, as shown inFIG. 1 , the rechargeable lithium battery may be a prismatic rechargeable lithium battery. - Referring to
FIG. 1 , arechargeable lithium battery 100 according to an embodiment may include anelectrode assembly 40 manufactured by winding aseparator 30 interposed between apositive electrode 10 and anegative electrode 20, and acase 50 housing theelectrode assembly 40. An electrolyte may be impregnated in thepositive electrode 10, thenegative electrode 20, and theseparator 30. The case may be sealed, for example, by a cover or cap or other form of sealing member, depending on the type of rechargeable lithium battery. Electrode tabs or terminals electrically connected to thepositive electrode 10 and thenegative electrode 20, respectively, may be outside the case. - The following Examples and Comparative Examples are provided in order to highlight characteristics of one or more embodiments, but it will be understood that the Examples and Comparative Examples are not to be construed as limiting the scope of the embodiments, nor are the Comparative Examples to be construed as being outside the scope of the embodiments. Further, it will be understood that the embodiments are not limited to the particular details described in the Examples and Comparative Examples.
- Lithium carbonate, nickel sulfate, cobalt sulfate, and manganese sulfate were mixed to have a mole ratio of Li:Ni:Co:Mn=1:0.5:0.2:0.3.
- The mixture was heat-treated at 740° C. under an oxygen (O2) atmosphere for 20 hours to prepare a LiNi0.5Co0.2Mn0.3O2 positive active material.
- 94 wt % of the prepared positive active material, 3 wt % of a polyvinylidene fluoride binder, and 3 wt % of a ketjen black conductive material were mixed or dissolved in an N-methylpyrrolidone solvent to prepare a positive active material composition. The positive active material composition was coated onto an Al current collector to manufacture a positive electrode.
- A LiNi0.6Co0.2Mn0.2O2 positive active material was prepared according to the same method as Experimental Example 1 except for mixing lithium carbonate, nickel sulfate, cobalt sulfate, and manganese sulfate to have a mole ratio of Li:Ni:Co:Mn=1:0.6:0.2:0.2. The positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- A LiNi0.7Co0.15Mn0.15O2 positive active material was prepared according to the same method as Experimental Example 1 except for mixing lithium hydroxide, nickel sulfate, cobalt sulfate, and manganese sulfate to have a mole ratio of Li:Ni:Co:Mn=1:0.7:0.15:0.15. The positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- A LiNi0.8Co0.15Al0.05O2 positive active material was prepared according to the same method as Experimental Example 1 except for mixing lithium hydroxide, nickel sulfate, cobalt sulfate, and aluminum sulfate to have a mole ratio of Li:Ni:Co:Al=1:0.8:0.15:0.05. The positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- A LiNi0.82Co0.15Al0.03O2 positive active material was prepared according to the same method as Experimental Example 1 except for mixing lithium hydroxide, nickel sulfate, cobalt sulfate, and aluminum sulfate to have a mole ratio of Li:Ni:Co:Al=1:0.82:0.15:0.03. The positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- A LiNi0.85Co0.135Al0.015O2 positive active material was prepared according to the same method as Experimental Example 1 except for mixing lithium hydroxide, nickel sulfate, cobalt sulfate, and aluminum sulfate to have a mole ratio of Li:Ni:Co:Al=1:0.85:0.135:0.015. The positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- A LiNi0.9Co0.09Al0.01O2 positive active material was prepared according to the same method as Experimental Example 1 except for mixing lithium hydroxide, nickel sulfate, cobalt sulfate, and aluminum sulfate to have a mole ratio of Li:Ni:Co:Al=1:0.9:0.09:0.01. The positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- A LiNi0.92Co0.07Al0.01O2 positive active material was prepared according to the same method as Experimental Example 1 except for mixing lithium hydroxide, nickel sulfate, cobalt sulfate, and aluminum sulfate to have a mole ratio of Li:Ni:Co:Al=1:0.92:0.07:0.01. The positive active material was used according to the same method as Experimental Example 1 to manufacture a positive electrode.
- Each positive electrode according to Experimental Examples 1 to 8, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method. The electrolyte was prepared by dissolving 1.0 M LiPF6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- The half-cell was charged and discharged at 25° C. within a range of 3.0 V to 4.3 V at 0.2 C. Then, the discharge capacity of the half-cell was measured. The results for Experimental Examples 1 to 8 are provided in
FIG. 2 . (The circles inFIG. 2 correspond to Experimental Examples 1 to 8 in order, from left to right.) - As shown in
FIG. 2 , as a nickel content was increased, capacity was increased. For example, when x in a LiaNixCoyMnzO2 compound was greater than or equal to 0.7 (greater than or equal to 70% inFIG. 2 ), a capacity greater than or equal to 180 mAh/g was obtained. - Lithium hydroxide, nickel sulfate, cobalt sulfate, and aluminum sulfate were mixed to have a mole ratio of Li:Ni:Co:Al:Ti=1:0.85:0.135:0.015.
- The mixture was primarily heat-treated at 740° C. under an oxygen (O2) atmosphere for 20 hours to prepare a LiNi0.85Co0.135Al0.015O2 core.
- The core was mixed with Co(OH)2 in a ratio of 100 wt %:1.5 wt % in a water solvent in a wet coating process, and the mixture was secondarily heat-treated at 700° C. under an oxygen atmosphere for 10 hours to prepare a positive active material including the LiNi0.85Co0.135Al0.015O2 core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core. The Co3O4 and LiaCoO2 structure-stabilizing compound was present as an island shape and a layered phase on the surface of the core. In addition, the structure-stabilizing compound was present in an amount of 1.5 wt % based on 100 wt % of the core in the final positive active material. 94 wt % of the prepared positive active material, 3 wt % of a polyvinylidene fluoride binder, and 3 wt % of a ketjen black conductive material were mixed or dissolved in an N-methylpyrrolidone solvent to prepare a positive active material composition. The positive active material composition was coated onto an Al current collector to manufacture a positive electrode.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Al0.015O2 core of Example 1 with Co(OH)2 in a ratio of 100 wt %:2 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 2 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Al0.015O2 core of Example 1 with Co(OH)2 in a ratio of 100 wt %:3 wt %. In the positive active material, the structure-stabilizing compound was present in an amount of 3 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Al0.015O2 core of Example 1 with Co(OH)2 in a ratio of 100 wt %:0.5 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 0.5 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Al0.015O2 core of Example 1 with Co(OH)2 in a ratio of 100 wt %:1 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 1 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Al0.015O2 core of Example 1 with Co(OH)2 in a ratio of 100 wt %:5 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 5 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
-
FIG. 3 illustrates a SEM image showing the positive active material of Example 1. As shown inFIG. 3 , the positive active material of Example 1 has a Co-including structure-stabilizing compound coated as an island shape and a layered phase on the surface of the core. -
FIG. 4(a) illustrates a TEM image showing the positive active material of Example 1,FIG. 4(b) illustrates a SAD (selected area diffraction) image showing the surface corresponding toarea 1 inFIG. 4(a) , andFIG. 4c ) ofFIG. 4 illustrates a SAD (selected area diffraction) image showing the surface corresponding toarea 2 in (FIG. 4a ). As shown inFIGS. 4(b) and 4(c) , the surface of the positive active material of Example 1 had a layered crystal structure and a mixed crystal structure. - Each positive electrode according to Examples 1 to 3 and Reference Examples 1 to 3, a lithium metal counter electrode, and an electrolyte were used to manufacture in a coin-type half-cell in a general method. The electrolyte was prepared by dissolving 1.3 M LiPF6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- The manufactured half-cell was charged and discharged 50 times at 25° C. in a range of 3.0 V to 4.3 V at 0.2 C, and discharge capacity of the half-cell was measured. In addition, a capacity retention was obtained by calculating a ratio of the 50th discharge capacity relative to the first discharge capacity as a cycle-life.
- The results of the half-cells respectively using the positive electrodes according to Examples 1 to 3 and Reference Examples 1 to 3 are shown in Table 1. In addition, the discharge capacity results of the half-cells respectively using the positive electrodes according to Examples 1 to 3 and Reference Examples 1 to 3 are shown in
FIG. 5 , and room temperature cycle-life characteristic results of the half-cells are shown inFIG. 6 . -
TABLE 1 Content of structure- Discharge Room temperature stabilizing compound capacity cycle-life (wt %) (mAh/g) (%) Reference 0.5 200 84 Example 1 Reference 1 200 84 Example 2 Example 1 1.5 200 85 Example 2 2 201 86 Example 3 3 201 87 Reference 5 199 83 Example 3 - As shown in Table 1 and
FIGS. 5 and 6 , the half-cells respectively using the positive electrodes using a positive active material including Co3O4 and LiaCoO2 as a structure-stabilizing compound in a range of 1.5 wt % to 3 wt % according to Examples 1 to 3 exhibited discharge capacity of greater than or equal to 200 mAh/g and cycle-life characteristics of greater than or equal to 85%. The half-cells including the structure-stabilizing compound in a smaller amount than the range according to Reference Examples 1 and 2 and the half-cells including the structure-stabilizing compound in a larger amount than the range according to Reference Example 3 exhibited deteriorated capacity and cycle-life characteristics. - Lithium hydroxide, nickel sulfate, cobalt sulfate, and aluminum sulfate were mixed to have a mole ratio of Li:Ni:Co:Al=1:0.85:0.135:0.015.
- The mixture was subjected to a primary heat treatment at 740° C. under an oxygen (O2) atmosphere for 20 hours to prepare a LiNi0.85Co0.135Al0.015O2 positive active material. A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- Each positive electrode according to Example 1 and Comparative Example 1, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method. The electrolyte was prepared by dissolving 1.3 M LiPF6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- The half-cells were charged and discharged once at 0.1 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm2 to perform a formation process. The charge and discharge capacities and efficiencies of the half-cells were measured, and the results are shown in Table 2.
- After the formation process, the cells were charged and discharged once at 0.2 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm2. The discharge capacities of the half cells were measured, and the results are shown in Table 2.
-
TABLE 2 Formation process 0.2 C 0.1 C charge 0.1 C discharge discharge capacity capacity Efficiency capacity (mAh/g) (mAh/g) (%) (mAh/g) Comparative 234.9 209.1 89.0 202.8 Example 1 Example 1 235.7 212.6 90.2 207.6 - As shown in Table 2, the positive active material having a structure-stabilizing compound on the surface according to Example 1 exhibited excellent charge and discharge characteristics compared with the positive active material including no structure-stabilizing compound according to Comparative Example 1.
- Lithium hydroxide, nickel sulfate, cobalt sulfate, and manganese sulfate were mixed to have a mole ratio of Li:Ni:Co:Mn=1:0.85:0.135:0.015.
- The mixture was subjected to a primary heat-treatment at 740° C. under an oxygen (O2) atmosphere for 20 hours to prepare a LiNi0.85Co0.135Mn0.015O2 core.
- The core was mixed with Co(OH)2 in a ratio of 100 wt %:1.5 wt % in a water solvent through a wet coating process, this mixture was subjected to a secondary heat-treatment at 700° C. under an oxygen atmosphere for 10 hours to prepare a positive active material including the LiNi0.85Co0.135Mn0.015O2 core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core. The Co3O4 and LiaCoO2 structure-stabilizing compound was present as an island shape and a layered phase on the surface of the core. In addition, in the final positive active material, the structure-stabilizing compound was included in an amount of 1.5 wt % based on 100 wt % of the core.
- 94 wt % of the prepared positive active material, 3 wt % of a polyvinylidene fluoride binder, and 3 wt % of a ketjen black conductive material were mixed or dissolved in an N-methylpyrrolidone solvent to prepare a positive active material composition. The positive active material composition was coated onto an Al current collector to manufacture a positive electrode.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Mn0.015O2 core of Example 4 with Co(OH)2 in a ratio of 100 wt %:2 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 2 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Mn0.015O2 core of Example 4 with Co(OH)2 in a ratio of 100 wt %:3 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 3 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Mn0.015O2 core of Example 4 with Co(OH)2 in a ratio of 100 wt %:0.5 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 0.5 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Mn0.015O2 core of Example 4 with Co(OH)2 in a ratio of 100 wt %:1 wt %. In the positive active material, the structure-stabilizing compound was present in an amount of 1 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- A positive active material including a core and a Co3O4 and LiaCoO2 (50:50 wt %, a=1.0) structure-stabilizing compound on the surface of the core was prepared according to the same method as Example 1 except for mixing the LiNi0.85Co0.135Mn0.015O2 core of Example 4 with Co(OH)2 in a ratio of 100 wt %:5 wt %. In the final positive active material, the structure-stabilizing compound was present in an amount of 5 wt % based on 100 wt % of the core.
- A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- Each positive electrode according to Examples 4 to 6 and Reference Examples 4 to 6, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method. The electrolyte was prepared by dissolving 1.3 M LiPF6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 of a volume ratio).
- The manufactured half-cells were charged and discharged 50 times at 25° C. in a range of 3.0 V to 4.3 Vat 0.2 C, and the discharge capacities of the half-cells were measured. In addition, a capacity retention value was obtained by calculating a ratio of the 50th discharge capacity relative to the first discharge capacity to evaluate a cycle-life.
- The results with respect to the half-cells manufactured by respectively using the positive electrodes according to Examples 4 to 6 and Reference Examples 4 to 6 were shown in Table 3.
-
TABLE 3 Content of structure- Discharge Room stabilizing compound capacity temperature (wt %) (mAh/g) cycle-life (%) Reference 0.5 200 84 Example 4 Reference 1 200 84 Example 5 Example 4 1.5 201 86 Example 5 2 202 87 Example 6 3 202 87 Reference 5 199 83 Example 6 - As shown in Table 3, the half-cells using the positive electrodes using the positive active material including Co3O4 and LiaCoO2 in an amount of 1.5 wt % to 3 wt % as a structure-stabilizing compound according to Examples 4 to 6 showed discharge capacity of greater than or equal to 200 mAh/g and cycle-life characteristics of greater than or equal to 85%, while the half-cells including the structure-stabilizing compound in a smaller amount than the range according to Reference Examples 4 and 5 and the half-cells including the structure-stabilizing compound in a larger amount than the range according to Reference Example 6 exhibited deteriorated cycle-life characteristics.
- Lithium hydroxide, nickel sulfate, cobalt sulfate, and manganese sulfate were mixed to have a mole ratio of Li:Ni:Co:Mn=1:0.85:0.135:0.015.
- The mixture was subjected to primary heat-treatment at 740° C. under an oxygen (O2) atmosphere for 20 hours to prepare a LiNi0.85Co0.135Mn0.015O2 positive active material. A positive electrode was manufactured using the positive active material according to the same method as in Example 1.
- Each positive electrode according to Example 4 and Comparative Example 2, a lithium metal counter electrode, and an electrolyte were used to manufacture a coin-type half-cell in a general method. The electrolyte was prepared by dissolving 1.3 M LiPF6 in a mixed solvent of ethylene carbonate and diethyl carbonate (50:50 volume ratio).
- The manufactured half-cells were charged and discharged once at 0.1 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm2 to perform a formation process. The charge and discharge capacities and efficiencies of the half-cells were obtained, and the results are shown in Table 4.
- In addition, after the formation process, the cells were charged and discharged once at 0.2 C in a range of 2.8 V to 4.4 V with a current density of 3.0 mA/cm2. The discharge capacities of the half-cells were obtained, and the results are shown in Table 4.
-
TABLE 4 Formation process 0.2 C 0.1 C charge 0.1 C discharge discharge capacity capacity Efficiency capacity (mAh/g) (mAh/g) (%) (mAh/g) Comparative 235.5 209.5 88.9 202.5 Example 2 Example 4 236.5 212.5 89.9 207.5 - As shown in Table 4, the positive active material having the structure-stabilizing compound on the surface according to Example 4 showed excellent charge and discharge characteristics compared with the positive active material including no structure-stabilizing compound according to Comparative Example 2.
- By way of summation and review, a rechargeable lithium battery includes a positive electrode, a negative electrode, and an electrolyte. A positive active material of a positive electrode may be an oxide including lithium and a transition metal and having a structure capable of intercalating lithium ions. For example, the positive active material may be LiCoO2, LiMn2O4, or LiNi1−xCoxO2 (0<x<1).
- As for a negative active material, various carbon-based materials such as artificial graphite, natural graphite, and hard carbon, which intercalate and deintercalate lithium ions.
- Recently, as mobile information terminals have been rapidly down-sized and made lighter, it has become desirable for a rechargeable lithium battery as an actuating power source to have a much higher capacity. In addition, in order to use the rechargeable lithium battery as an actuating power source or as a power storage source for a hybrid vehicle or an electric vehicle, research on developing a battery having a satisfactory high rate capability, an ability to be rapidly charged and discharged, and excellent cycle characteristics is being actively conducted.
- Embodiments provide a positive active material for a rechargeable lithium battery having high capacity and excellent cycle-life characteristics.
- Embodiment provide a rechargeable lithium battery including the positive active material.
- Example embodiments have been disclosed herein, and although specific terms are employed, they are used and are to be interpreted in a generic and descriptive sense only and not for purpose of limitation. In some instances, as would be apparent to one of ordinary skill in the art as of the filing of the present application, features, characteristics, and/or elements described in connection with a particular embodiment may be used singly or in combination with features, characteristics, and/or elements described in connection with other embodiments unless otherwise specifically indicated. Accordingly, it will be understood by those of skill in the art that various changes in form and details may be made without departing from the spirit and scope thereof as set forth in the following claims.
Claims (5)
1.-8. (canceled)
9. A positive active material formed by a process comprising:
mixing a core including a compound represented by Chemical Formula 1 and Co(OH)2 in a water solvent, and
heat-treating the mixture at about 500° C. to about 800° C. for about 5 to about 20 hours, thereby preparing the positive active material,
LiaNixCoyMezM1 kO2−pFp [Chemical Formula 1]
LiaNixCoyMezM1 kO2−pFp [Chemical Formula 1]
wherein, 0.9≤a≤1.1, 0.7≤x≤0.93, 0<y≤0.3, 0≤z≤0.3, 0≤k≤0.005, x+y+z+k=1, 0 p≤0.005,
Me is Mn or Al, and
M1 is Mg, Ba, B, La, Y, Ti, Zr, Mn, Si, V, P, Mo, W, or a combination thereof.
10. The positive active material as claimed in claim 9 , wherein mixing the core including the compound represented by Chemical Formula 1 and Co(OH)2 includes mixing Co(OH)2 in an amount of about 1.5 wt % to about 3 wt % based on 100 wt % of the core.
11. The positive active material as claimed in claim 9 , wherein heat-treating the mixture is at 700° C. under an oxygen atmosphere for 10 hours.
12. The positive active material as claimed in claim 9 , wherein the positive active material prepared by the process includes the core and Co3O4 and LiaCoO2 on the surface of the core.
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US15/487,635 US10637042B2 (en) | 2016-04-15 | 2017-04-14 | Positive active material for rechargeable lithium battery and rechargeable lithium battery including same |
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KR20190048923A (en) | 2017-10-31 | 2019-05-09 | 울산과학기술원 | Cathode active material for lithium ion secondary batteries, method for manufacturing the same, and lithium ion secondary batteries including the same |
KR20220084283A (en) * | 2019-10-22 | 2022-06-21 | 바스프 에스이 | Electrode active material and method of manufacturing the electrode active material |
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