CN114709370B - 一种凝胶相金属锂负极的固态电池 - Google Patents
一种凝胶相金属锂负极的固态电池 Download PDFInfo
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- CN114709370B CN114709370B CN202210410224.4A CN202210410224A CN114709370B CN 114709370 B CN114709370 B CN 114709370B CN 202210410224 A CN202210410224 A CN 202210410224A CN 114709370 B CN114709370 B CN 114709370B
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- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 66
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 42
- 229910052751 metal Inorganic materials 0.000 title claims abstract description 18
- 239000002184 metal Substances 0.000 title claims abstract description 18
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 43
- 238000003756 stirring Methods 0.000 claims abstract description 20
- 239000002904 solvent Substances 0.000 claims abstract description 17
- 150000003839 salts Chemical class 0.000 claims abstract description 14
- 239000000203 mixture Substances 0.000 claims abstract description 12
- 239000006258 conductive agent Substances 0.000 claims abstract description 10
- 229920001940 conductive polymer Polymers 0.000 claims abstract description 9
- 239000007787 solid Substances 0.000 claims abstract description 8
- 239000002390 adhesive tape Substances 0.000 claims abstract description 7
- 239000007774 positive electrode material Substances 0.000 claims abstract 4
- 239000000463 material Substances 0.000 claims description 37
- 238000003466 welding Methods 0.000 claims description 24
- 229910052782 aluminium Inorganic materials 0.000 claims description 16
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical group [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 16
- 229920000642 polymer Polymers 0.000 claims description 13
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 12
- ZUOUZKKEUPVFJK-UHFFFAOYSA-N diphenyl Chemical compound C1=CC=CC=C1C1=CC=CC=C1 ZUOUZKKEUPVFJK-UHFFFAOYSA-N 0.000 claims description 12
- -1 lithium nickel cobalt aluminum Chemical compound 0.000 claims description 10
- 238000005096 rolling process Methods 0.000 claims description 10
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 claims description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 9
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 9
- 239000002033 PVDF binder Substances 0.000 claims description 9
- 239000011230 binding agent Substances 0.000 claims description 9
- 229910052802 copper Inorganic materials 0.000 claims description 9
- 239000010949 copper Substances 0.000 claims description 9
- 239000011261 inert gas Substances 0.000 claims description 9
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 9
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 claims description 8
- 239000011245 gel electrolyte Substances 0.000 claims description 8
- 238000005520 cutting process Methods 0.000 claims description 7
- 239000011259 mixed solution Substances 0.000 claims description 7
- 238000012545 processing Methods 0.000 claims description 7
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 6
- 239000004743 Polypropylene Substances 0.000 claims description 6
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 claims description 6
- MWPLVEDNUUSJAV-UHFFFAOYSA-N anthracene Chemical compound C1=CC=CC2=CC3=CC=CC=C3C=C21 MWPLVEDNUUSJAV-UHFFFAOYSA-N 0.000 claims description 6
- 239000004305 biphenyl Substances 0.000 claims description 6
- 235000010290 biphenyl Nutrition 0.000 claims description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 6
- 229920002239 polyacrylonitrile Polymers 0.000 claims description 6
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 6
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 6
- ZUHZGEOKBKGPSW-UHFFFAOYSA-N tetraglyme Chemical compound COCCOCCOCCOCCOC ZUHZGEOKBKGPSW-UHFFFAOYSA-N 0.000 claims description 6
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 5
- 239000002985 plastic film Substances 0.000 claims description 5
- 229920006255 plastic film Polymers 0.000 claims description 5
- 229920000058 polyacrylate Polymers 0.000 claims description 5
- 238000006116 polymerization reaction Methods 0.000 claims description 5
- UUAMLBIYJDPGFU-UHFFFAOYSA-N 1,3-dimethoxypropane Chemical compound COCCCOC UUAMLBIYJDPGFU-UHFFFAOYSA-N 0.000 claims description 4
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 claims description 4
- RYHBNJHYFVUHQT-UHFFFAOYSA-N 1,4-Dioxane Chemical compound C1COCCO1 RYHBNJHYFVUHQT-UHFFFAOYSA-N 0.000 claims description 4
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 claims description 4
- 238000005516 engineering process Methods 0.000 claims description 4
- 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 4
- 229920003229 poly(methyl methacrylate) Polymers 0.000 claims description 4
- 229920005569 poly(vinylidene fluoride-co-hexafluoropropylene) Polymers 0.000 claims description 4
- 229920001197 polyacetylene Polymers 0.000 claims description 4
- 229920000767 polyaniline Polymers 0.000 claims description 4
- 239000004926 polymethyl methacrylate Substances 0.000 claims description 4
- 229920000123 polythiophene Polymers 0.000 claims description 4
- 239000002203 sulfidic glass Substances 0.000 claims description 4
- BJEWLOAZFAGNPE-UHFFFAOYSA-N 1-ethenylsulfonylethane Chemical compound CCS(=O)(=O)C=C BJEWLOAZFAGNPE-UHFFFAOYSA-N 0.000 claims description 3
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 3
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 claims description 3
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 claims description 3
- 229920003171 Poly (ethylene oxide) Polymers 0.000 claims description 3
- 239000004698 Polyethylene Substances 0.000 claims description 3
- GOOHAUXETOMSMM-UHFFFAOYSA-N Propylene oxide Chemical compound CC1CO1 GOOHAUXETOMSMM-UHFFFAOYSA-N 0.000 claims description 3
- 229920002125 Sokalan® Polymers 0.000 claims description 3
- 229910000831 Steel Inorganic materials 0.000 claims description 3
- DHXVGJBLRPWPCS-UHFFFAOYSA-N Tetrahydropyran Chemical compound C1CCOCC1 DHXVGJBLRPWPCS-UHFFFAOYSA-N 0.000 claims description 3
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 claims description 3
- 239000004917 carbon fiber Substances 0.000 claims description 3
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 3
- 239000002041 carbon nanotube Substances 0.000 claims description 3
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 claims description 3
- NKDDWNXOKDWJAK-UHFFFAOYSA-N dimethoxymethane Chemical compound COCOC NKDDWNXOKDWJAK-UHFFFAOYSA-N 0.000 claims description 3
- FFHWGQQFANVOHV-UHFFFAOYSA-N dimethyldioxirane Chemical compound CC1(C)OO1 FFHWGQQFANVOHV-UHFFFAOYSA-N 0.000 claims description 3
- 239000002223 garnet Substances 0.000 claims description 3
- 229910021389 graphene Inorganic materials 0.000 claims description 3
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 3
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 3
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 3
- 238000002844 melting Methods 0.000 claims description 3
- 230000008018 melting Effects 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- AHHWIHXENZJRFG-UHFFFAOYSA-N oxetane Chemical compound C1COC1 AHHWIHXENZJRFG-UHFFFAOYSA-N 0.000 claims description 3
- 238000004806 packaging method and process Methods 0.000 claims description 3
- KFSLWBXXFJQRDL-UHFFFAOYSA-N peroxyacetic acid Substances CC(=O)OO KFSLWBXXFJQRDL-UHFFFAOYSA-N 0.000 claims description 3
- 229920000128 polypyrrole Polymers 0.000 claims description 3
- 239000004814 polyurethane Substances 0.000 claims description 3
- 229920002635 polyurethane Polymers 0.000 claims description 3
- 239000010959 steel Substances 0.000 claims description 3
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 claims description 3
- 239000002253 acid Substances 0.000 claims 1
- 239000004760 aramid Substances 0.000 claims 1
- 229920003235 aromatic polyamide Polymers 0.000 claims 1
- AZMFPLDNKPTEIA-UHFFFAOYSA-N ethene;ethenyl hydrogen sulfite Chemical compound C=C.OS(=O)OC=C AZMFPLDNKPTEIA-UHFFFAOYSA-N 0.000 claims 1
- 238000004519 manufacturing process Methods 0.000 abstract description 12
- 210000001787 dendrite Anatomy 0.000 abstract description 4
- 230000008021 deposition Effects 0.000 abstract description 2
- 239000000853 adhesive Substances 0.000 abstract 1
- 230000001070 adhesive effect Effects 0.000 abstract 1
- 238000007599 discharging Methods 0.000 abstract 1
- 229910001338 liquidmetal Inorganic materials 0.000 abstract 1
- 238000000034 method Methods 0.000 description 12
- 238000010438 heat treatment Methods 0.000 description 10
- 239000007788 liquid Substances 0.000 description 7
- 239000013543 active substance Substances 0.000 description 6
- 239000001307 helium Substances 0.000 description 6
- 229910052734 helium Inorganic materials 0.000 description 6
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 6
- 239000012528 membrane Substances 0.000 description 6
- 239000011248 coating agent Substances 0.000 description 5
- 238000000576 coating method Methods 0.000 description 5
- 238000001125 extrusion Methods 0.000 description 5
- 239000002202 Polyethylene glycol Substances 0.000 description 4
- 238000004146 energy storage Methods 0.000 description 4
- 239000011244 liquid electrolyte Substances 0.000 description 4
- 229910001416 lithium ion Inorganic materials 0.000 description 4
- YNPNZTXNASCQKK-UHFFFAOYSA-N phenanthrene Chemical compound C1=CC=C2C3=CC=CC=C3C=CC2=C1 YNPNZTXNASCQKK-UHFFFAOYSA-N 0.000 description 4
- OZAIFHULBGXAKX-UHFFFAOYSA-N 2-(2-cyanopropan-2-yldiazenyl)-2-methylpropanenitrile Chemical compound N#CC(C)(C)N=NC(C)(C)C#N OZAIFHULBGXAKX-UHFFFAOYSA-N 0.000 description 3
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 238000001816 cooling Methods 0.000 description 3
- 239000011888 foil Substances 0.000 description 3
- 238000009998 heat setting Methods 0.000 description 3
- 229920000671 polyethylene glycol diacrylate Polymers 0.000 description 3
- 238000007789 sealing Methods 0.000 description 3
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- WNLXKBDXIAGXQA-UHFFFAOYSA-N [Cl].[P].[S].[Li] Chemical compound [Cl].[P].[S].[Li] WNLXKBDXIAGXQA-UHFFFAOYSA-N 0.000 description 2
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 description 2
- 229920006231 aramid fiber Polymers 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 150000002148 esters Chemical class 0.000 description 2
- RBBXSUBZFUWCAV-UHFFFAOYSA-N ethenyl hydrogen sulfite Chemical compound OS(=O)OC=C RBBXSUBZFUWCAV-UHFFFAOYSA-N 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 238000009966 trimming Methods 0.000 description 2
- NRJJZXGPUXHHTC-UHFFFAOYSA-N [Li+].[O--].[O--].[O--].[O--].[Zr+4].[La+3] Chemical compound [Li+].[O--].[O--].[O--].[O--].[Zr+4].[La+3] NRJJZXGPUXHHTC-UHFFFAOYSA-N 0.000 description 1
- XRNHBMJMFUBOID-UHFFFAOYSA-N [O].[Zr].[La].[Li] Chemical compound [O].[Zr].[La].[Li] XRNHBMJMFUBOID-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 125000004386 diacrylate group Chemical group 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- CEMTZIYRXLSOGI-UHFFFAOYSA-N lithium lanthanum(3+) oxygen(2-) titanium(4+) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Ti+4].[La+3] CEMTZIYRXLSOGI-UHFFFAOYSA-N 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 229920000867 polyelectrolyte Polymers 0.000 description 1
- 229920001223 polyethylene glycol Polymers 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
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
- H01M4/13—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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—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
- H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
-
- 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
- H01M10/058—Construction or manufacture
- H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
-
- 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
-
- 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
- H01M4/381—Alkaline or alkaline earth metals elements
- H01M4/382—Lithium
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
- H01M4/622—Binders being polymers
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
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- H—ELECTRICITY
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- H01M2004/023—Gel electrode
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0082—Organic polymers
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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
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- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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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
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Abstract
一种凝胶相金属锂负极的固态电池,由凝胶相锂金属负极片、正极片、外壳组成,先将金属锂或者导电盐放入基础溶剂中,然后再加入聚合溶剂、导电聚合物搅拌均匀,将凝胶相锂混合物涂抹在集流体上,压平,用隔膜袋包裹,再将隔膜袋上口焊接在集流体上即得到凝胶相金属锂负极片;正极片由正极活性物质、导电剂、粘结剂、固态电解质、集流体组成,将制造好的正极片和凝胶相金属锂负极按设定的数量堆叠起来,用胶布困扎好,焊接正极耳、负极耳,装上外壳,将极耳连接到外壳上制造出成品。该电池金属锂以凝胶相存在,可以改善固态锂金属和固态电解质界面接触电阻大、充放电过程中剥离沉积易分层塌陷以及枝晶的问题,还能解决液体金属锂负极不好制造成片状极片的问题。
Description
技术领域
本发明涉及固态电池领域,尤其是一种凝胶相金属锂负极的固态电池。
背景技术
新能源电池行业已在国内发展多年,其市场规模已在全球范围内首屈一指,是国民经济的一个重要组成部分,同时也发展出全球领先的龙头企业。但目前动力电池仍然存在短板,电池自燃原因有很多,但液态电解液的运用是其中一大弊端,其主要由有机溶剂组成,很容易燃烧,在电池遇到特殊情况时液态电解液无疑起到推波助澜作用。
固态电池由于主要采用非液体电解质,从而改善了常规液态电池易燃易爆炸的安全问题。经多方测试认证采用非液态的准固态和固态电池均能通过针刺试验,电池安全性能得到了大幅提高。固态电池已成为未来电池的发展方向,目前各大相关科研机构和企业都在进行固态电池研究,目前业内排名靠前的企业都已布局固态电池业务。虽然固态电池如火如荼的发展了多年,但目前仍然没有达到量产的条件。究其原因主要有负极锂金属运用工艺不成熟以及固态电解质层和正负极副反应过多等。负极金属在充放电过程中沉积和剥离时容易和固态电解质隔离层发生脱离和塌陷,迅速恶化电池性能。同时固态电解质隔离层和正极间存在空间电荷层增大了接触阻抗,导致锂离子导通困难。还有固态电解质尤其时硫化物固态电解质对环境和溶剂要求很高,很难适配,另外锂金属仍然会在固态电解质层中形成锂枝晶,等等。有人曾经尝试采用液态锂金属负极来制造金属锂负极电池,但电池的体积比能量和质量比能很低,还不如常规液态电池。还有电池要想大规模量产必须要像现在一样将电池正负极做成片状才有利于批量化生产,而这些对于液态锂负极来说无疑是灾难性的。
发明内容
本发明的目的是提供一种凝胶相金属锂负极的固态电池,解决固态电池负极锂金属在沉积剥离过程中容易塌陷和固态电解质层分离问题、液态锂负极不好制造成片状问题以及固态电解质和正极片之间容易形成空间电荷层问题。
本发明的目的是以如下方式实现的:一种凝胶相金属锂负极的固态电池,由凝胶相锂金属负极片、正极片、外壳组成,先在真空或者惰性气体保护环境下,将金属锂或者导电盐放入基础溶剂中,搅拌溶解,然后再加入聚合溶剂、导电聚合物搅拌均匀,将混合液放入真空或者惰性气体保护环境下,40-60℃放置6-24小时,取出将凝胶相锂混合物涂抹在集流体上,压平,用隔膜袋包裹,再将隔膜袋上口焊接在集流体上即得到凝胶相金属锂负极片;外壳可以铝塑膜、铝壳或钢壳,电池加工工艺为:将制造好的正极片和凝胶相金属锂负极按设定的数量堆叠起来,用胶布困扎好,然后将正极耳焊接在一起,负极耳焊接在一起,装上外壳,将极耳连接到外壳上,封装外壳,化成分容后就制造出本发明电池。
正极片由正极活性物质、导电剂、粘结剂、固态电解质、集流体组成,其中正极活性物质由钴酸锂、镍钴锰酸锂、镍钴铝酸锂、富锂锰、锰酸锂、磷酸铁锂等材料中的至少一种材料组成,导电剂由导电炭黑、碳纳米管、石墨烯、碳纤维材料中至少一种组成,粘结剂由PVDF、PTFE、PAA、PAN中至少一种组成,固态电解质由硫化物固态电解质、石榴石型固态电解质、钙钛矿型固态电解质、LISCON型固态电解质、聚合物固态电解质中至少一种组成,集流体为铝材,8-13um厚,生产时先将正极活性物质、导电剂、粘结剂、固态电解质混合均匀,然后用辊轧机轧成薄片,然后将薄片放置到集流体上加热加压复合到一起,然后分切成小片状。
基础溶剂为苯、联苯、萘、蒽、菲、乙二醇二甲醚、四乙二醇二甲醚、1,3-丙二醇二甲醚中的至少两种。
聚合溶剂为1、3-二氧戊环、甲缩醛、环氧乙烷、1 ,4-二氧六环、环氧丙烷、四氢呋喃、二甲基二环氧乙烷、三甲撑氧、四氢吡喃中的至少一种。
负极集流体为铜材料,4-12um厚度,上面开有若干通孔,顶部留白作极片极耳用。
隔膜袋的隔膜由基材、聚合物固态电解质、凝胶电解质、导电盐、微量碳酸脂组成,先将聚合物固态电解质和基材按混合熔融挤出拉伸工艺制成多孔状隔膜体,孔隙率在60-70%,将导电盐、微量碳酸脂加入凝胶电解质搅拌均匀,真空或者惰性气体保护下,40-60℃,搁置6-24小时,然后涂抹到隔膜体上,刮平,裁切成方形,对折,将底边和侧边焊接在一起;基材为PP、PE、PVDF、芳纶、聚氨酯中的至少一种,聚合物固态电解质为PEO、PAN、PVDF、PMMA中的至少一种,凝胶电解质为PAN-MMA 、PVDF-HFP 、ETPTA 、PEGDA、乙烯基亚硫酸乙烯酯、碳酸乙烯亚乙酯、聚丙烯酸酯、乙基乙烯基砜中的至少一种,导电盐为LiClO4、LiPF6、LiBF6、LiAsF6、LiFTSI、LiBOB、LiBF4、LiDFOB中的至少一种,微量碳酸脂为EC、PC、DMC、DEC、EMC中的至少一种。
导电聚合物为聚乙炔、聚苯胺、聚噻吩、聚吡咯、聚吲哚中的至少一种。
本发明电池由凝胶相金属锂负极片、正极片、外壳组成,负极锂采用凝胶态,其优点是凝胶态物质不但可以溶解锂,还可以和固态电解质层保持柔性接触,保持相界不脱离,避免锂枝晶形成和界面塌陷问题形成。联苯、乙二醇二甲醚等溶剂可以溶解锂金属,起到存储锂的作用,譬如锂可以[(Bp·-) Li+](C4H10O2)形式存在,并且Li+可以移动。另外我们把醚类原位聚合电解液混合到上文的溶液中,同时加入导电盐、导电聚合物,混合均匀,然后加热后形成凝胶。而该凝胶本身具有锂离子导通功能,再加上导电盐的作用,凝胶电导率大幅提升。导电聚合物主要用来引入电子,导电聚合物可以和集流体连接使整个凝胶内都可以得到或者输出电子。预先溶解的少量锂可以引导整个凝胶体系的容锂活性。
然后将常规隔膜、氧化物固态电解质和聚合物固态电解质、导电盐做成多孔复合隔离膜,在孔中填上凝胶,凝胶中添加导电盐并吸入少量溶剂,这样既保证了隔离膜的韧性,又保持了良好的锂离子导电性,同时可以和正极片保持柔性连接,消除了空间电荷层。
本发明的电池由于金属锂以凝胶相存在,不但可以改善固态锂金属和固态电解质界面接触电阻大、充放电过程中剥离沉积易分层塌陷以及枝晶等问题,而且能解决液体金属锂负极不好制造成片状极片的问题。本发明制造的全固态电池循环寿命长、倍率性能好,可裁切成任意形状,加工工艺简单,制造成本低,很好地推动了固态电池发展。
附图说明
图1是本发明凝胶相金属锂负极片的结构示意图。
图2是本发明300Ah铝壳储能电池放电曲线图。
图3是本发明300Ah铝壳储能电池循环寿命图。
图4是本发明100Ah软包动力电池放电曲线图。
图5是本发明100Ah软包动力电池循环寿命图。
图6是本发明6Ah手机电池放电曲线图。
图7是本发明6Ah手机电池循环寿命图。
具体实施方式
参照图1,一种凝胶相金属锂负极的固态电池,由凝胶相锂金属负极片、正极片、外壳组成,先在真空或者惰性气体保护环境下,将金属锂或者导电盐放入基础溶剂中,搅拌溶解,然后再加入聚合溶剂、导电聚合物搅拌均匀,将混合液放入真空或者惰性气体保护环境下,40-60℃放置6-24小时,取出将凝胶相锂混合物涂抹在集流体上,压平,用隔膜袋包裹,再将隔膜袋上口焊接在集流体上即得到凝胶相金属锂负极片;外壳可以铝塑膜、铝壳或钢壳,电池加工工艺为:将制造好的正极片和凝胶相金属锂负极按设定的数量堆叠起来,用胶布困扎好,然后将正极耳焊接在一起,负极耳焊接在一起,装上外壳,将极耳连接到外壳上,封装外壳,化成分容后就制造出本发明电池。
正极片由正极活性物质、导电剂、粘结剂、固态电解质、集流体组成,其中正极活性物质由钴酸锂、镍钴锰酸锂、镍钴铝酸锂、富锂锰、锰酸锂、磷酸铁锂等材料中的至少一种材料组成,导电剂由导电炭黑、碳纳米管、石墨烯、碳纤维材料中至少一种组成,粘结剂由PVDF、PTFE、PAA、PAN中至少一种组成,固态电解质由硫化物固态电解质、石榴石型固态电解质、钙钛矿型固态电解质、LISCON型固态电解质、聚合物固态电解质中至少一种组成,集流体为铝材,8-13um厚,生产时先将正极活性物质、导电剂、粘结剂、固态电解质混合均匀,然后用辊轧机轧成薄片,然后将薄片放置到集流体上加热加压复合到一起,然后分切成小片状。
基础溶剂为苯、联苯、萘、蒽、菲、乙二醇二甲醚、四乙二醇二甲醚、1,3-丙二醇二甲醚中的至少两种。
聚合溶剂为1、3-二氧戊环、甲缩醛、环氧乙烷、1 ,4-二氧六环、环氧丙烷、四氢呋喃、二甲基二环氧乙烷、三甲撑氧、四氢吡喃中的至少一种。
负极集流体为铜材料,4-12um厚度,上面开有若干通孔,顶部留白作极片极耳用。
隔膜袋的隔膜由基材、聚合物固态电解质、凝胶电解质、导电盐、微量碳酸脂组成,先将聚合物固态电解质和基材按混合熔融挤出拉伸工艺制成多孔状隔膜体,孔隙率在60-70%,将导电盐、微量碳酸脂加入凝胶电解质搅拌均匀,真空或者惰性气体保护下,40-60℃,搁置6-24小时,然后涂抹到隔膜体上,刮平,裁切成方形,对折,将底边和侧边焊接在一起;基材为PP、PE、PVDF、芳纶、聚氨酯中的至少一种,聚合物固态电解质为PEO、PAN、PVDF、PMMA中的至少一种,凝胶电解质为PAN-MMA 、PVDF-HFP 、ETPTA 、PEGDA、乙烯基亚硫酸乙烯酯、碳酸乙烯亚乙酯、聚丙烯酸酯、乙基乙烯基砜中的至少一种,导电盐为LiClO4、LiPF6、LiBF6、LiAsF6、LiFTSI、LiBOB、LiBF4、LiDFOB中的至少一种,微量碳酸脂为EC、PC、DMC、DEC、EMC中的至少一种。
导电聚合物为聚乙炔、聚苯胺、聚噻吩、聚吡咯、聚吲哚中的至少一种。实施例1
用本发明方法制造300Ah铝壳储能电池。
露点低于-55℃,氦气保护下,取29.552千克联苯、34.554千克乙二醇二甲醚放入搅拌釜搅拌30分钟,加入0.104千克锂搅拌1小时,然后分别取14.2千克1、3-二氧戊环、0.8千克六氟磷酸锂、0.8千克聚乙炔加入搅拌釜,搅拌2小时,将混合液放入烘箱,抽真空,60℃加热8小时,取出,在露点低于-55℃、氦气保护环境下,将凝胶涂抹在铜网上,压平,面密度71.933克/平米,铜网极耳处留白,裁切成料区115mm×524mm。
隔膜加工:取3千克PP、4千克PEO,混合后按熔融挤出、高倍率拉伸、冷却、热处理、拉伸、热定型、分切、收卷等工艺做成68%孔隙率12um厚度的隔膜。露点低于-55℃,取1.7千克PEGDA(聚乙二醇双丙烯酸酯)、1千克锂镧锆氧、0.6千克六氟磷酸锂、30克偶氮二异丁腈、15克EC、15克DMC加入搅拌釜搅拌均匀,然后放入烘箱,抽真空,60℃加热8小时获得隔膜凝胶;取已制好多孔隔膜,将隔膜凝胶涂抹在隔膜上,每面10um。裁切成238mm×534mm,对折后对齐,用热封焊将底边、侧边焊接在一起,包裹在负极片上,然后将顶部焊接在集流体上。
取26.7千克经LAGP包覆的三元材料、0.9千克PTFE、0.6千克SP、0.3千克碳、1.5千克锂镧锆氧加入搅拌釜搅拌均匀,用辊轧机轧成200克/平米面密度61um厚薄片,然后将薄片铺平到铝箔上,夹到加热板中间,调整压力2吨,加热80℃,保温2小时,取出,冷却后裁切成料区112mm×520mm。
取36片正极片、37片正极片,依次叠成方块状,正极片在负极片正中间,最后上下面一块是负极片,用胶布将方块捆好,用超声波焊接机将正极耳焊到一起、负极耳焊到一起;取铝壳,将叠芯装配到壳内,装两块,然后装支架,焊连接片,激光封口,再化成分容后就得到本发明300Ah固态储能电池。
电池放电曲线图和电池循环寿命图参见图2、图3。
实施例2
用本发明方法制造100Ah软包动力电池。
露点低于-55℃,氦气保护下,取25.823千克萘、36.314千克乙二醇二甲醚放入搅拌釜搅拌30分钟,加入0.112千克锂搅拌1小时,然后分别取17.752千克1、4-二氧六环、0.8千克六氟磷酸锂、0.8千克聚苯胺加入搅拌釜,搅拌2小时,将混合液放入烘箱,抽真空,60℃加热8小时;取出,在露点低于-55℃、氦气保护环境下,将凝胶涂抹在铜网上,压平,面密度61.687克/平米,铜网极耳处留白,裁切成料区115mm×524mm。
隔膜加工:取3千克PP、4千克PMMA,混合后按熔融挤出、高倍率拉伸、冷却、热处理、拉伸、热定型、分切、收卷等工艺做成66%孔隙率12um厚度的隔膜;露点低于-55℃,取1.6千克碳酸乙烯亚乙酯、0.1千克聚丙烯酸酯、1千克锂镧钛氧、0.6千克六氟磷酸锂、30克偶氮二异丁腈、15克EC、15克DMC加入搅拌釜搅拌均匀,然后放入烘箱,抽真空,60℃加热8小时获得隔膜凝胶;取已制好多孔隔膜,将隔膜凝胶涂抹在隔膜上,每面10um,裁切成238mm×534mm,对折后对齐,用热封焊将底边、侧边焊接在一起,包裹在负极片上,然后将顶部焊接在集流体上。
取26.7千克经LAGP包覆的三元材料、0.9千克PTFE、0.6千克SP、0.3千克碳、1.5千克锂磷硫氯加入搅拌釜搅拌均匀,用辊轧机轧成180克/平米面密度61um厚薄片,然后将薄片铺平到铝箔上,夹到加热板中间,调整压力2吨,加热80℃,保温2小时;取出,冷却后裁切成料区115mm×524mm。
取39片正极片、40片正极片,依次叠成方块状,正极片在负极片正中间,最后上下面一块是负极片;用胶布将方块捆好,用超声波焊接机将正极耳焊到一起、负极耳焊到一起;取冲好的铝塑膜外壳,将叠芯装配到壳内,热封,修边,再化成二封,最后分容后就得到本发明100Ah动力电池。
电池放电曲线图和电池循环寿命图参见图4、图5。
实施例3
用本发明方法制造6Ah手机电池。
露点低于-55℃,氦气保护下,取28.241千克联苯、38.091千克1、3-丙二醇二甲醚放入搅拌釜搅拌30分钟,加入0.104千克锂搅拌1小时,然后分别取0.8千克六氟磷酸锂、聚噻吩加入搅拌釜,搅拌2小时,交混合液放入烘箱,抽真空,60℃加热8小时;取出,在露点低于-55℃、氦气保护环境下,将凝胶涂抹在铜网上,压平,面密度98.384克/平米,铜网极耳处留白,裁切成料区64mm×130mm。
隔膜加工:取3千克PP、4千克PVDF-HFP,混合后按熔融挤出、高倍率拉伸、冷却、热处理、拉伸、热定型、分切、收卷等工艺做成62%孔隙率12um厚度的隔膜;露点低于-55℃,取1.6千克碳酸乙烯亚乙酯、0.1千克聚丙烯酸酯、1千克锂铝锗磷、0.6千克六氟磷酸锂、30克偶氮二异丁腈、15克EC、15克DMC加入搅拌釜搅拌均匀,然后放入烘箱,抽真空,60℃加热8小时获得隔膜凝胶;取已制好多孔隔膜,将隔膜凝胶涂抹在隔膜上,每面10um;裁切成136mm×140mm,对折后对齐,用热封焊将底边、侧边焊接在一起,包裹在负极片上,然后将顶部焊接在集流体上。
取26.7千克富锂锰、0.9千克PTFE、0.6千克SP、0.3千克碳、1.5千克锂磷硫氯加入搅拌釜搅拌均匀,用辊轧机轧成200克/平米面密度61um厚薄片,然后将薄片铺平到铝箔上,夹到加热板中间,调整压力2吨,加热80℃,2小时。取出,冷却后裁切成料区100mm×550mm。
取8片正极片、9片正极片,依次叠成方块状,正极片在负极片正中间,最后上下面一块是负极片;用胶布将方块捆好,用超声波焊接机将正极耳焊到一起、负极耳焊到一起;取冲好的铝塑膜外壳,将叠芯装配到壳内,热封,修边,再化成二封,最后分容后就得到本发明6Ah手机电池。
电池放电曲线图和电池循环寿命图参见图6、图7。
Claims (4)
1.一种凝胶相金属锂负极的固态电池,由凝胶相锂金属负极片、正极片、外壳组成;先在真空或者惰性气体保护环境下,将金属锂放入基础溶剂中,搅拌溶解,然后再加入聚合溶剂、导电聚合物搅拌均匀,将混合液放入真空或者惰性气体保护环境下,40-60℃放置6-24小时,取出将凝胶相锂混合物涂抹在集流体上,压平,用隔膜袋包裹,再将隔膜袋上口焊接在集流体上即得到凝胶相金属锂负极片;基础溶剂为苯、联苯、萘、蒽、菲中的至少一种和乙二醇二甲醚、四乙二醇二甲醚、1,3-丙二醇二甲醚中的至少一种的混合物;正极片由正极活性物质、导电剂、粘结剂、固态电解质、集流体组成,其中正极活性物质由钴酸锂、镍钴锰酸锂、镍钴铝酸锂、富锂锰、锰酸锂或磷酸铁锂中的至少一种材料组成,导电剂由导电炭黑、碳纳米管、石墨烯或碳纤维材料中至少一种组成,粘结剂由PVDF、PTFE、PAA或PAN中至少一种组成,固态电解质由硫化物固态电解质、石榴石型固态电解质、钙钛矿型固态电解质、LISCON型固态电解质或聚合物固态电解质中至少一种组成,集流体为铝材,8-13um厚,生产时先将正极活性物质、导电剂、粘结剂、固态电解质混合均匀,然后用辊轧机轧成薄片,然后将薄片放置到集流体上加热加压复合到一起,然后分切成小片状;隔膜袋的隔膜由基材、聚合物固态电解质、凝胶电解质、导电盐、微量碳酸脂,先将聚合物固态电解质和基材按混合熔融挤出拉伸工艺制成多孔状隔膜体,孔隙率在60-70%,将导电盐、微量碳酸脂加入凝胶电解质搅拌均匀,真空或者惰性气体保护下,40-60℃,搁置6-24小时,然后涂抹到隔膜体上,刮平,裁切成方形,对折,将底边和侧边焊接在一起;基材为PP、PE、PVDF、芳纶或聚氨酯中的至少一种,聚合物固态电解质为PEO、PAN、PVDF或PMMA中的至少一种,凝胶电解质为PAN-MMA、PVDF-HFP 、ETPTA 、PEGDA、乙烯基亚硫酸乙烯酯、碳酸乙烯亚乙酯、聚丙烯酸酯或乙基乙烯基砜中的至少一种,导电盐为LiClO4、LiPF6、LiBF6、LiAsF6、LiFTSI、LiBOB、LiBF4或LiDFOB中的至少一种,微量碳酸脂为EC、PC、DMC、DEC或EMC中的至少一种;外壳为铝塑膜、铝壳或钢壳,电池加工工艺为:将制造好的正极片和凝胶相金属锂负极按设定的数量堆叠起来,用胶布困扎好,然后将正极耳焊接在一起,负极耳焊接在一起,装上外壳,将极耳连接到外壳上,封装外壳,化成分容后就制造出该固态电池。
2.根据权利要求1所述的一种凝胶相金属锂负极的固态电池,其特征在于:聚合溶剂为1、3-二氧戊环、甲缩醛、环氧乙烷、1 ,4-二氧六环、环氧丙烷、四氢呋喃、二甲基二环氧乙烷、三甲撑氧或四氢吡喃中的至少一种。
3.根据权利要求1所述的一种凝胶相金属锂负极的固态电池,其特征在于:负极集流体为铜材料,4-12um厚度,上面开有若干通孔,顶部留白作极片极耳用。
4.根据权利要求1所述的一种凝胶相金属锂负极的固态电池,其特征在于:导电聚合物为聚乙炔、聚苯胺、聚噻吩、聚吡咯或聚吲哚中的至少一种。
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