WO2012036519A2 - 마그네슘 이차전지용 전극 및 이를 구비한 마그네슘 이차전지 - Google Patents
마그네슘 이차전지용 전극 및 이를 구비한 마그네슘 이차전지 Download PDFInfo
- Publication number
- WO2012036519A2 WO2012036519A2 PCT/KR2011/006880 KR2011006880W WO2012036519A2 WO 2012036519 A2 WO2012036519 A2 WO 2012036519A2 KR 2011006880 W KR2011006880 W KR 2011006880W WO 2012036519 A2 WO2012036519 A2 WO 2012036519A2
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- Prior art keywords
- electrode
- magnesium
- secondary battery
- group
- magnesium secondary
- Prior art date
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- 239000011777 magnesium Substances 0.000 title claims abstract description 101
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 title claims abstract description 96
- 229910052749 magnesium Inorganic materials 0.000 title claims abstract description 94
- 238000004519 manufacturing process Methods 0.000 claims abstract description 15
- 238000007747 plating Methods 0.000 claims description 38
- 238000000034 method Methods 0.000 claims description 27
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 claims description 26
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 14
- 239000003792 electrolyte Substances 0.000 claims description 14
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 claims description 13
- 159000000003 magnesium salts Chemical class 0.000 claims description 12
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 11
- 125000004432 carbon atom Chemical group C* 0.000 claims description 10
- 229910052802 copper Inorganic materials 0.000 claims description 10
- 239000010949 copper Substances 0.000 claims description 10
- 239000000243 solution Substances 0.000 claims description 9
- 125000000217 alkyl group Chemical group 0.000 claims description 8
- 229910052736 halogen Inorganic materials 0.000 claims description 8
- 229910052782 aluminium Inorganic materials 0.000 claims description 7
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 claims description 6
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 6
- 229910052759 nickel Inorganic materials 0.000 claims description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 5
- 239000003575 carbonaceous material Substances 0.000 claims description 5
- DHKHKXVYLBGOIT-UHFFFAOYSA-N 1,1-Diethoxyethane Chemical compound CCOC(C)OCC DHKHKXVYLBGOIT-UHFFFAOYSA-N 0.000 claims description 4
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 claims description 4
- 125000004448 alkyl carbonyl group Chemical group 0.000 claims description 4
- 125000003277 amino group Chemical group 0.000 claims description 4
- 125000003118 aryl group Chemical group 0.000 claims description 4
- 229910052804 chromium Inorganic materials 0.000 claims description 4
- 239000011651 chromium Substances 0.000 claims description 4
- 239000002131 composite material Substances 0.000 claims description 4
- 239000000203 mixture Substances 0.000 claims description 4
- 239000003960 organic solvent Substances 0.000 claims description 4
- 229910052720 vanadium Inorganic materials 0.000 claims description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 3
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 claims description 3
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 3
- 239000007818 Grignard reagent Substances 0.000 claims description 3
- 239000008151 electrolyte solution Substances 0.000 claims description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 3
- 229910052742 iron Inorganic materials 0.000 claims description 3
- 229910052751 metal Inorganic materials 0.000 claims description 3
- 239000002184 metal Substances 0.000 claims description 3
- 229910044991 metal oxide Inorganic materials 0.000 claims description 3
- 150000004706 metal oxides Chemical class 0.000 claims description 3
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- SJHAYVFVKRXMKG-UHFFFAOYSA-N 4-methyl-1,3,2-dioxathiolane 2-oxide Chemical compound CC1COS(=O)O1 SJHAYVFVKRXMKG-UHFFFAOYSA-N 0.000 claims description 2
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 2
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 2
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 2
- 239000006182 cathode active material Substances 0.000 claims description 2
- 229910017052 cobalt Inorganic materials 0.000 claims description 2
- 239000010941 cobalt Substances 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 2
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 claims description 2
- 150000004795 grignard reagents Chemical class 0.000 claims description 2
- 150000004820 halides Chemical class 0.000 claims description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 2
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052750 molybdenum Inorganic materials 0.000 claims description 2
- 239000011733 molybdenum Substances 0.000 claims description 2
- 229910052707 ruthenium Inorganic materials 0.000 claims description 2
- 229910052706 scandium Inorganic materials 0.000 claims description 2
- SIXSYDAISGFNSX-UHFFFAOYSA-N scandium atom Chemical compound [Sc] SIXSYDAISGFNSX-UHFFFAOYSA-N 0.000 claims description 2
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 claims description 2
- 229910052719 titanium Inorganic materials 0.000 claims description 2
- 229910052725 zinc Inorganic materials 0.000 claims description 2
- 239000011701 zinc Substances 0.000 claims description 2
- 125000005843 halogen group Chemical group 0.000 claims 2
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims 1
- 125000000472 sulfonyl group Chemical group *S(*)(=O)=O 0.000 claims 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims 1
- 239000010409 thin film Substances 0.000 abstract description 8
- 239000010410 layer Substances 0.000 description 18
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 12
- 229910052744 lithium Inorganic materials 0.000 description 12
- 239000011888 foil Substances 0.000 description 10
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 6
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 6
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 description 6
- 229910052794 bromium Inorganic materials 0.000 description 6
- 229910052801 chlorine Inorganic materials 0.000 description 6
- 239000000460 chlorine Substances 0.000 description 6
- 150000002367 halogens Chemical group 0.000 description 6
- JLVVSXFLKOJNIY-UHFFFAOYSA-N Magnesium ion Chemical compound [Mg+2] JLVVSXFLKOJNIY-UHFFFAOYSA-N 0.000 description 5
- 239000011889 copper foil Substances 0.000 description 5
- 229910001425 magnesium ion Inorganic materials 0.000 description 5
- 239000002904 solvent Substances 0.000 description 5
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical group [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 4
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 4
- 239000005977 Ethylene Substances 0.000 description 4
- 239000011230 binding agent Substances 0.000 description 4
- 229910052799 carbon Inorganic materials 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 239000004020 conductor Substances 0.000 description 4
- 229920001577 copolymer Polymers 0.000 description 4
- QUXHCILOWRXCEO-UHFFFAOYSA-M magnesium;butane;chloride Chemical compound [Mg+2].[Cl-].CCC[CH2-] QUXHCILOWRXCEO-UHFFFAOYSA-M 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- 229910017267 Mo 6 S 8 Inorganic materials 0.000 description 3
- 125000004390 alkyl sulfonyl group Chemical group 0.000 description 3
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 3
- 239000011247 coating layer Substances 0.000 description 3
- 238000002484 cyclic voltammetry Methods 0.000 description 3
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 3
- 125000004674 methylcarbonyl group Chemical group CC(=O)* 0.000 description 3
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 3
- 229920006254 polymer film Polymers 0.000 description 3
- 239000007774 positive electrode material Substances 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 125000001889 triflyl group Chemical group FC(F)(F)S(*)(=O)=O 0.000 description 3
- PAYRUJLWNCNPSJ-UHFFFAOYSA-N Aniline Chemical compound NC1=CC=CC=C1 PAYRUJLWNCNPSJ-UHFFFAOYSA-N 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 2
- -1 aluminum Chemical class 0.000 description 2
- 125000002490 anilino group Chemical group [H]N(*)C1=C([H])C([H])=C([H])C([H])=C1[H] 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 150000002739 metals Chemical class 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- YCWSUKQGVSGXJO-NTUHNPAUSA-N nifuroxazide Chemical group C1=CC(O)=CC=C1C(=O)N\N=C\C1=CC=C([N+]([O-])=O)O1 YCWSUKQGVSGXJO-NTUHNPAUSA-N 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
- 150000003623 transition metal compounds Chemical class 0.000 description 2
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 239000006245 Carbon black Super-P Substances 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- 229910020599 Co 3 O 4 Inorganic materials 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 125000005234 alkyl aluminium group Chemical group 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- IAQRGUVFOMOMEM-UHFFFAOYSA-N butene Natural products CC=CC IAQRGUVFOMOMEM-UHFFFAOYSA-N 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000011267 electrode slurry Substances 0.000 description 1
- 238000007772 electroless plating Methods 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 125000005678 ethenylene group Chemical group [H]C([*:1])=C([H])[*:2] 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229920001519 homopolymer Polymers 0.000 description 1
- 229910001416 lithium ion Inorganic materials 0.000 description 1
- 229910003002 lithium salt Inorganic materials 0.000 description 1
- 159000000002 lithium salts Chemical class 0.000 description 1
- 150000002681 magnesium compounds Chemical class 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 229920002239 polyacrylonitrile Polymers 0.000 description 1
- 239000004926 polymethyl methacrylate Substances 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 229920001384 propylene homopolymer Polymers 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 238000007634 remodeling Methods 0.000 description 1
- 239000012266 salt solution Substances 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 150000004763 sulfides Chemical class 0.000 description 1
- 238000001771 vacuum deposition Methods 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0438—Processes of manufacture in general by electrochemical processing
-
- 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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
-
- 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
-
- 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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
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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
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
-
- 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
- H01M4/04—Processes of manufacture in general
- H01M4/0438—Processes of manufacture in general by electrochemical processing
- H01M4/045—Electrochemical coating; Electrochemical impregnation
- H01M4/0452—Electrochemical coating; Electrochemical impregnation from solutions
-
- 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
- H01M4/134—Electrodes based on metals, Si or alloys
-
- 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
- H01M4/139—Processes of manufacture
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Definitions
- the present invention relates to a magnesium secondary battery electrode and a magnesium secondary battery having the same. More specifically, the present invention relates to a magnesium secondary battery electrode and a magnesium secondary battery having the same, which can be easily manufactured in a thin film structure at low cost.
- Lithium secondary batteries As a battery capable of satisfying such a demand, lithium secondary batteries developed in the early 1990s are widely used. Lithium secondary batteries are manufactured in which a non-aqueous electrolyte solution in which lithium salt is appropriately dissolved in a positive electrode and a mixed organic solvent made of a negative electrode such as a carbon material capable of occluding and releasing lithium ions, a lithium-containing oxide, and the like is provided in a battery case.
- lithium secondary batteries have a safety problem due to side reactions of the electrolyte and high reactivity of lithium, and lithium element is expensive because it is not resource-rich.
- these safety and cost problems of the lithium secondary battery has become a matter to be considered more recently with the increase in the demand for medium and large batteries has become an obstacle to using a lithium secondary battery as a medium and large battery.
- Magnesium secondary batteries are secondary batteries that can be charged and discharged by moving electrons as magnesium ions are inserted into and desorbed from the positive electrode active material using an electrode, specifically, a magnesium plate as a negative electrode, and magnesium has a theoretical capacity density similar to that of lithium.
- it is attracting attention as a battery that can replace a lithium secondary battery because it is environmentally friendly, inexpensive than lithium and superior in terms of battery safety.
- magnesium plate used as a cathode is lower than that of lithium, but not lower than that of other metals.
- the thickness of the negative electrode should be thinned, and the thin plate of magnesium should be made.
- Magnesium has a low formability compared to other metals such as aluminum, and thus requires a high level of technology to manufacture thin plates, resulting in a high process cost. There is a problem that rises, it remains a problem in the commercialization of magnesium secondary batteries.
- an object of the present invention is to provide a magnesium secondary battery electrode having a thin film structure which can increase the energy density of a battery at low cost, and a magnesium secondary battery having the same.
- the electrode for magnesium secondary battery of the present invention the current collector; And a magnesium plating layer formed on the surface of the current collector.
- the electrode may be a cathode.
- the magnesium plating layer may have a thickness of 1 ⁇ m to 20 ⁇ m, but is not limited thereto.
- the magnesium plating layer according to the present invention may be formed by electrochemical plating.
- the current collector may be made of copper, aluminum, steal use stainless (SUS), nickel or a carbon-based material.
- the manufacturing method of the electrode for magnesium secondary batteries of the present invention (S1) a working electrode, a counter electrode (counter electrode) and a reference electrode (reference electrode) in a solution in which magnesium salt is dissolved Dipping; (S2) applying a voltage to the electrodes; And (S3) obtaining an electrode having a magnesium plating layer formed on the current collector, which is the main electrode.
- the magnesium salt is RMgX (R is a straight or branched alkyl group having 1 to 10 carbon atoms, a straight or branched aryl group having 1 to 10 carbon atoms, or a straight or branched amine group having 1 to 10 carbon atoms.
- X is halogen and preferably chlorine or bromine
- MgX 2 is halogen and preferably chlorine or bromine
- R 2 Mg R Silver alkyl group, dialkyl boron group, diaryl boron group, alkyl carbonyl group (for example methylcarbonyl group (-CO 2 CH 3 )) or alkylsulfonyl group (for example trifluoromethylsulfonyl group (-SO 2 CF 3 )) and MgClO 4 may be used alone or in combination of two or more thereof.
- the electrode for magnesium secondary batteries of the present invention can be usefully used for the production of magnesium secondary batteries having high energy density.
- Magnesium secondary battery electrode of the present invention is a simple manufacturing process compared to the magnesium foil or magnesium ribbon used as a conventional magnesium secondary battery electrode, it is possible to lower the manufacturing cost by using easily obtainable copper foil or aluminum foil as a current collector have.
- the thickness of the magnesium plating layer can be freely adjusted, it is possible to manufacture the electrode as needed.
- a thin film electrode can be manufactured, a magnesium secondary battery having a high energy density can be manufactured.
- FIG. 1 is a photograph of an electrode for a magnesium secondary battery manufactured according to an embodiment of the present invention.
- FIG. 2 is an XRD measurement graph of an electrode for a magnesium secondary battery manufactured according to an embodiment of the present invention.
- FIG 3 is a cyclic voltammetry graph of a three-electrode cell using a magnesium secondary battery electrode prepared according to an embodiment of the present invention.
- Figure 4 is a graph of the charge and discharge test results of the coin cell prepared according to Example 3 and Comparative Example 1.
- Magnesium secondary battery electrode of the present invention is a current collector; And a magnesium plating layer formed on the surface of the current collector.
- the electrode according to the present invention may be a cathode.
- the current collector according to the present invention can be used without limitation as long as it is an electrically conductive conductor.
- copper or aluminum having excellent electrical conductivity and formability and low cost may be used in the form of a foil or a ribbon. .
- the magnesium plating layer according to the present invention is a magnesium coating layer formed on the surface of the current collector by a conventional plating method.
- the magnesium plating layer according to the present invention may have a thickness of 1 ⁇ m to 20 ⁇ m, preferably 1 ⁇ m to 15 ⁇ m, and more preferably 1 ⁇ m to 10 ⁇ m, but is not limited thereto.
- the method of plating magnesium on the current collector is not particularly limited as long as it is a plating method capable of forming a plating layer in a uniform thin film structure.
- a wet plating method and a dry plating method may be applied.
- the wet plating method may be an electrochemical plating method, an electroless plating method, or the like
- the dry plating method may be a vacuum deposition method, a sputtering method, or the like. It is not.
- the manufacturing method to be described is a manufacturing method based on the electrochemical plating method, but the plating method that can be applied to the present invention as described above is various, the method described below is merely an example and the scope of the present invention is not limited thereto.
- the main electrode, the counter electrode and the reference electrode are immersed in a solution in which magnesium salt is dissolved.
- Magnesium salts that may be used include RMgX (R is a straight or branched alkyl group having 1 to 10 carbon atoms, a straight or branched aryl group having 1 to 10 carbon atoms, or a straight or branched chain having 1 to 10 carbon atoms.
- Amine group preferably methyl group, ethyl group, butyl group, phenyl group, or aniline group
- X is halogen, preferably chlorine or bromine
- MgX 2 X is halogen, preferably chlorine or bromine
- R 2 Mg R is an alkyl group, a dialkyl boron group, a diaryl boron group, an alkylcarbonyl group (eg methylcarbonyl group (-CO 2 CH 3 )) or an alkylsulfonyl group (eg trifluoromethylsulfonyl group (-SO 2 CF 3 )
- MgClO 4 and the like may be used alone or in combination of two or more, and may be used by mixing alkyl aluminum as an additive.
- magnesium salt is dissolved in a suitable solvent
- any solvent may be used as long as it can dissolve the compound.
- organic solvents such as tetrahydrofuran (THF).
- the current collector When the magnesium salt solution is prepared, a working electrode, a counter electrode and a reference electrode are immersed in the solution. At this time, it is preferable that the current collector according to the present invention is used as the main electrode.
- the current collector may be a foil or a ribbon made of copper, aluminum, steal use stainless (SUS), nickel or a carbon-based material (for example, carbon paper, carbon fiber, carbon seed, etc.).
- An electrode made of magnesium may be used as the reference electrode, and a platinum electrode may be used as the counter electrode.
- the thickness of the magnesium plating layer applied on the current collector can be freely adjusted by adjusting the concentration of the magnesium salt or the plating time.
- the electrode manufactured as described above may be usefully used for a magnesium secondary battery.
- the electrode may be a cathode.
- the magnesium secondary battery may include an electrode, a separator, and an electrolyte solution prepared as described above.
- the magnesium secondary battery may include a cathode, a cathode prepared as described above, a separator interposed between the anode and the cathode, and an electrolyte solution.
- the positive electrode of the magnesium secondary battery according to the present invention may be manufactured by a manufacturing method commonly used in the art.
- a cathode may be prepared by mixing and stirring a binder and a solvent, a conductive material and a dispersant, as necessary, and then applying it to a current collector and compressing the cathode active material.
- transition metal compound or a magnesium composite metal oxide capable of inserting / desorcing magnesium ions may be used as the positive electrode active material.
- transition metal compounds include oxides, sulfides or halides such as scandium, ruthenium, titanium, vanadium, molybdenum, chromium, manganese, iron, cobalt, nickel, copper, zinc, and more specifically, TiS 2 , ZrS 2 , RuO 2 , Co 3 O 4 , Mo 6 S 8 , V 2 O 5, and the like may be used, but is not limited thereto.
- examples of the magnesium composite metal oxide include Mg (M 1-x A x ) O 4 (0 ⁇ x ⁇ 0.5, M is Ni, Co, Mn, Cr, V, Fe, Cu, or Ti, and A is Al, B , Si, Cr, V, C, Na, K or Mg) may be used a magnesium compound.
- Binders include vinylidene fluoride-hexafluoropropylene copolymer (PVDF-co-HFP), polyvinylidene fluoride, polyacrylonitrile, polymethylmethacrylate, and the like. Kinds of binder polymers may be used.
- Conductive carbon is commonly used as the conductive material, and for example, various conductive carbon materials such as graphite, carbon black, acetylene black, caten black, denka black, super-P, and carbon nanotubes may be used.
- a magnesium secondary battery may be manufactured by interposing a separator between the positive electrode and the negative electrode and including an electrolyte.
- the electrolyte used in the present invention is required to be an electrochemically stable electrolyte at 1V or more relative to magnesium for stable operation of the battery.
- magnesium salt may be used as the electrolyte used in the electrolyte, and for example, a Grignard reagent compound prepared with Grignard reagent, which is a strong reducing agent, may be used. More specifically, RMgX (R may be 1 to C).
- X is halogen, preferably chlorine or bromine
- MgX 2 X is halogen and preferably chlorine or bromine
- R 2 Mg R is alkyl group, dialkylboron group, diarylboron Group, alkylcarbonyl group (e.g. methylcarbonyl group (-CO 2 CH 3 )) or alkylsulfonyl group (e.g. trifluoromethylsulfonyl group (-SO 2 CF 3 )), MgClO 4 and the like, respectively Or mixed two or more
- the present invention is not limited thereto.
- a solvent capable of dissolving the electrolyte as a solvent used in the electrolyte, for example, propylene carbonate (PC), ethylene carbonate (EC), di Ethyl carbonate (DEC), dimethyl carbonate (DMC), ethylmethyl carbonate (EMC), methylpropyl carbonate, dipropyl carbonate, dimethylsulfuroxide, acetonitrile, dimethoxyethane, diethoxyethane, vinylene
- PC propylene carbonate
- EC ethylene carbonate
- DEC di Ethyl carbonate
- DMC dimethyl carbonate
- EMC ethylmethyl carbonate
- methylpropyl carbonate dipropyl carbonate
- dimethylsulfuroxide acetonitrile
- dimethoxyethane diethoxyethane
- separator conventional inorganic separators or organic separators conventionally used as separators may be used.
- a glass filter may be used as the inorganic separator, and a porous polymer film may be used as the organic separator.
- the porous polymer film is, for example, alone or a porous polymer film made of a polyolefin-based polymer such as ethylene homopolymer, propylene homopolymer, ethylene / butene copolymer, ethylene / hexene copolymer and ethylene / methacrylate copolymer, or the like. These can be laminated
- the battery case used in the present invention may be adopted that is commonly used in the art, there is no limitation on the appearance according to the use of the battery, for example, cylindrical, square, pouch type or coin using a can (coin) type and the like.
- the plating layer is uniformly formed on the copper current collector.
- the peaks of magnesium and copper can be confirmed, respectively, from which a magnesium coating layer is formed on the copper current collector.
- the amount of plated magnesium was about 0.0022g, the thickness of the plated layer was about 3 ⁇ m.
- a three-electrode magnesium battery was prepared using the electrode prepared according to Example 1 as a negative electrode (relative electrode). Mo 6 S 8 was used as the positive electrode (main electrode), magnesium foil was used as the reference electrode, and 0.25M Mg (AlCl 2 BuEt) 2 solution dissolved in tetrahydrofuran was used as the electrolyte.
- Cyclic voltammetry of the prepared battery was measured at room temperature (scan rate: 100 Hz / s), and the results are shown in FIG. 3.
- the electrode of the present invention can be usefully used as an electrode for a magnesium secondary battery (eg, a negative electrode) since the insertion-tally peak of magnesium ions appears in the graph.
- a magnesium secondary battery eg, a negative electrode
- Mo 6 S 8 as a positive electrode active material, Denka black as a conductive material, and KF1100 as a binder were added to NMP at a ratio of 80:10:10 and mixed to prepare a positive electrode slurry, followed by 10 ⁇ m thick SUS. It was applied to the foil and dried to prepare a positive electrode.
- a glass filter was used as a separator between the anode and the prepared anode, and a coin cell using a 0.25 M Mg (AlCl 2 BuEt) 2 solution dissolved in tetrahydrofuran as an electrolyte. was prepared.
- a coin cell was manufactured in the same manner as in Example 3, except that 50 ⁇ m thick thin film magnesium foil was used as the cathode.
- Example 3 and Comparative Example 1 prepared above were charged and discharged at 0.3 V to 1.8 V with 0.1 C-rate, and a voltage profile and a capacity were measured. The results are shown in FIG. 4.
- the magnesium is inserted in the 0.1C charge and discharge remodeling of Example 3, the capacity is also about 80 mAh / g, it is confirmed that the level equivalent to Comparative Example 1 using a magnesium thin film foil used as a conventional negative electrode Can be.
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Abstract
Description
Claims (13)
- 집전체; 및상기 집전체 표면에 형성된 마그네슘 도금층;을 포함하는 마그네슘 이차전지용 전극.
- 제1항에 있어서,상기 전극은 음극인 것을 특징으로 하는 마그네슘 이차전지용 전극.
- 제1항에 있어서,상기 마그네슘 도금층은 1㎛ 내지 20㎛의 두께를 갖는 것을 특징으로 하는 마그네슘 이차전지용 전극.
- 제1항에 있어서,상기 마그네슘 도금층은 전기화학적 도금에 의해 형성되는 것을 특징으로 하는 마그네슘 이차전지용 전극.
- 제1항에 있어서,상기 집전체는 구리, 알루미늄, SUS(steal use stainless), 니켈 또는 탄소계 물질을 포함하는 것을 특징으로 하는 마그네슘 이차전지용 전극.
- 마그네슘염이 용해된 용액에 주전극, 상대전극 및 기준전극을 침지하는 단계;상기 전극들에 전압을 인가하는 단계; 및상기 주전극인 집전체 상에 마그네슘 도금층이 형성된 전극을 얻는 단계를 포함하는 마그네슘 이차전지용 전극의 제조방법.
- 제6항에 있어서,상기 주전극은 전지의 집전체인 것을 특징으로 하는 마그네슘 이차전지용 전극의 제조방법.
- 제6항에 있어서,상기 마그네슘염은 RMgX(R은 탄소수 1 내지 10인 직쇄형이거나 분지형의 탄소수 1 내지 10인 직쇄형이거나 분지형의 알킬기, 탄소수 1 내지 10인 직쇄형이거나 분지형의 아릴기, 또는 탄소수 1 내지 10인 직쇄형이거나 분지형의 아민기이며, X는 할로겐임), MgX2 (X는 할로겐임), R2Mg (R은 알킬기, 디알킬보론기, 디아릴보론기, 알킬카보닐기 또는 알킬설포닐기임), 및 MgClO4 로 이루어진 군에서 선택되는 어느 하나 또는 이들 중 2종 이상의 혼합물을 포함하는 것을 특징으로 하는 마그네슘 이차전지용 전극의 제조방법.
- 양극, 음극, 상기 양극과 음극 사이에 개재된 세퍼레이터 및 전해액을 구비한 마그네슘 이차전지에 있어서,상기 음극은 제1항 내지 제5항 중 어느 한 항의 전극인 것을 특징으로 하는 마그네슘 이차전지.
- 제9항에 있어서,상기 양극은 스칸듐, 루테늄, 티타늄, 바나듐, 몰리브덴, 크롬, 망간, 철, 코발트, 니켈, 구리 및 아연으로 이루어진 군에서 선택되는 금속의 산화물, 황화물 또는 할로겐화물; 및 마그네슘 복합금속 산화물로 이루어진 군에서 선택되는 어느 하나 또는 이들 중 2종 이상의 혼합물인 양극 활물질을 구비하는 것을 특징으로 하는 마그네슘 이차전지.
- 제9항에 있어서,상기 전해액은 마그네슘 대비 1V 이상에서 전기화학적으로 안정한 것을 특징으로 하는 마그네슘 이차전지.
- 제9항에 있어서,상기 전해액은 그리냐르 시약계 합성물을 포함하는 전해질을 구비하는 것을 특징으로 하는 마그네슘 이차전지.
- 제9항에 있어서,상기 전해액은 프로필렌 카보네이트, 에틸렌 카보네이트, 디에틸 카보네이트, 디메틸 카보네이트, 에틸메틸 카보네이트, 메틸프로필 카보네이트, 디프로필 카보네이트, 디메틸설퍼옥사이드, 아세토니트릴, 디메톡시에탄, 디에톡시에탄, 비닐렌 카보네이트, 설포란, 감마-부티로락톤, 프로필렌 설파이트 및 테트라하이드로푸란으로 이루어진 군에서 선택되는 어느 하나 또는 이들 중 2종 이상의 혼합물인 유기용매를 구비하는 것을 특징으로 하는 마그네슘 이차전지.
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CN2011800042456A CN102714298A (zh) | 2010-09-17 | 2011-09-16 | 用于镁二次电池的电极及包括该电极的镁二次电池 |
EP11825479.6A EP2472647A4 (en) | 2010-09-17 | 2011-09-16 | ELECTRODE FOR A RECHARGEABLE MAGNESIUM BATTERY AND RECHARGEABLE MAGNESIUM BATTERY THEREOF |
JP2012534131A JP2012531725A (ja) | 2010-09-17 | 2011-09-16 | マグネシウム二次電池用電極及びこれを備えたマグネシウム二次電池 |
US13/827,633 US20130196236A1 (en) | 2010-09-17 | 2013-03-14 | Electrode for magnesium secondary battery and magnesium secondary battery including the same |
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KR1020110093448A KR101302076B1 (ko) | 2010-09-17 | 2011-09-16 | 마그네슘 이차전지용 전극 및 이를 구비한 마그네슘 이차전지 |
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JP5162822B2 (ja) * | 2005-12-02 | 2013-03-13 | ソニー株式会社 | 電気化学デバイス |
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JP5076321B2 (ja) * | 2006-01-12 | 2012-11-21 | ソニー株式会社 | 電池 |
JP2007280627A (ja) * | 2006-04-03 | 2007-10-25 | Matsushita Electric Ind Co Ltd | マグネシウム二次電池 |
US9012072B2 (en) * | 2007-01-25 | 2015-04-21 | Bar-Ilan University | Rechargeable magnesium battery |
WO2008120162A2 (en) * | 2007-04-02 | 2008-10-09 | Koninklijke Philips Electronics N.V. | Electrochemical energy source and electronic device provided with such an electrochemical energy source |
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2011
- 2011-09-16 WO PCT/KR2011/006880 patent/WO2012036519A2/ko active Application Filing
- 2011-09-16 CN CN2011800042456A patent/CN102714298A/zh active Pending
- 2011-09-16 EP EP11825479.6A patent/EP2472647A4/en not_active Withdrawn
- 2011-09-16 JP JP2012534131A patent/JP2012531725A/ja active Pending
- 2011-09-16 KR KR1020110093448A patent/KR101302076B1/ko active IP Right Grant
-
2013
- 2013-03-14 US US13/827,633 patent/US20130196236A1/en not_active Abandoned
-
2014
- 2014-05-07 JP JP2014096270A patent/JP6066956B2/ja active Active
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None |
See also references of EP2472647A4 |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US10073490B2 (en) | 2011-07-29 | 2018-09-11 | Sony Corporation | Display and electronic unit |
Also Published As
Publication number | Publication date |
---|---|
KR101302076B1 (ko) | 2013-09-05 |
JP6066956B2 (ja) | 2017-01-25 |
KR20120030021A (ko) | 2012-03-27 |
EP2472647A4 (en) | 2013-07-03 |
JP2014179336A (ja) | 2014-09-25 |
JP2012531725A (ja) | 2012-12-10 |
CN102714298A (zh) | 2012-10-03 |
EP2472647A2 (en) | 2012-07-04 |
US20130196236A1 (en) | 2013-08-01 |
WO2012036519A3 (ko) | 2012-06-28 |
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