CN117219879A - Non-negative electrode lithium ion battery and preparation method thereof - Google Patents
Non-negative electrode lithium ion battery and preparation method thereof Download PDFInfo
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- CN117219879A CN117219879A CN202311257180.7A CN202311257180A CN117219879A CN 117219879 A CN117219879 A CN 117219879A CN 202311257180 A CN202311257180 A CN 202311257180A CN 117219879 A CN117219879 A CN 117219879A
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- positive electrode
- lithium
- negative electrode
- solid electrolyte
- ion battery
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 66
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 66
- 238000002360 preparation method Methods 0.000 title claims abstract description 22
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 100
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 57
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 51
- 239000011267 electrode slurry Substances 0.000 claims abstract description 47
- 239000011230 binding agent Substances 0.000 claims abstract description 38
- 229910052751 metal Inorganic materials 0.000 claims abstract description 31
- 239000002184 metal Substances 0.000 claims abstract description 31
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 18
- 230000001502 supplementing effect Effects 0.000 claims abstract description 17
- 239000002994 raw material Substances 0.000 claims abstract description 14
- 239000006258 conductive agent Substances 0.000 claims description 18
- 239000007774 positive electrode material Substances 0.000 claims description 17
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 15
- 239000003792 electrolyte Substances 0.000 claims description 15
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 15
- 239000002904 solvent Substances 0.000 claims description 14
- 239000002033 PVDF binder Substances 0.000 claims description 10
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 10
- 238000006136 alcoholysis reaction Methods 0.000 claims description 8
- 238000000034 method Methods 0.000 claims description 7
- FVXHSJCDRRWIRE-UHFFFAOYSA-H P(=O)([O-])([O-])[O-].[Ge+2].[Al+3].[Li+].P(=O)([O-])([O-])[O-] Chemical compound P(=O)([O-])([O-])[O-].[Ge+2].[Al+3].[Li+].P(=O)([O-])([O-])[O-] FVXHSJCDRRWIRE-UHFFFAOYSA-H 0.000 claims description 4
- 239000000654 additive Substances 0.000 claims description 4
- 239000007787 solid Substances 0.000 claims description 4
- 229910018068 Li 2 O Inorganic materials 0.000 claims description 3
- 229920003171 Poly (ethylene oxide) Polymers 0.000 claims description 3
- 230000000996 additive effect Effects 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
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 3
- 239000013589 supplement Substances 0.000 claims description 3
- CVJYOKLQNGVTIS-UHFFFAOYSA-K aluminum;lithium;titanium(4+);phosphate Chemical compound [Li+].[Al+3].[Ti+4].[O-]P([O-])([O-])=O CVJYOKLQNGVTIS-UHFFFAOYSA-K 0.000 claims description 2
- WVDJDYHWHDLSAZ-UHFFFAOYSA-N [O].[Ti].[La].[Li] Chemical compound [O].[Ti].[La].[Li] WVDJDYHWHDLSAZ-UHFFFAOYSA-N 0.000 claims 1
- KZGIKPHEKSDETK-UHFFFAOYSA-N [O].[Ti].[Zr].[La].[Li] Chemical compound [O].[Ti].[Zr].[La].[Li] KZGIKPHEKSDETK-UHFFFAOYSA-N 0.000 claims 1
- XRNHBMJMFUBOID-UHFFFAOYSA-N [O].[Zr].[La].[Li] Chemical compound [O].[Zr].[La].[Li] XRNHBMJMFUBOID-UHFFFAOYSA-N 0.000 claims 1
- 239000013543 active substance Substances 0.000 abstract description 2
- 230000002427 irreversible effect Effects 0.000 abstract description 2
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 24
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 14
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 12
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 description 12
- 210000001787 dendrite Anatomy 0.000 description 11
- 230000000052 comparative effect Effects 0.000 description 10
- 238000006243 chemical reaction Methods 0.000 description 9
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 9
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 8
- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical compound COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 description 8
- 230000008021 deposition Effects 0.000 description 7
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 6
- 229910000664 lithium aluminum titanium phosphates (LATP) Inorganic materials 0.000 description 6
- 229910003870 O—Li Inorganic materials 0.000 description 5
- 239000000853 adhesive Substances 0.000 description 5
- 230000001070 adhesive effect Effects 0.000 description 5
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 description 5
- 125000000524 functional group Chemical group 0.000 description 5
- 150000002500 ions Chemical class 0.000 description 5
- -1 lithium hexafluorophosphate Chemical compound 0.000 description 5
- HNAGHMKIPMKKBB-UHFFFAOYSA-N 1-benzylpyrrolidine-3-carboxamide Chemical compound C1C(C(=O)N)CCN1CC1=CC=CC=C1 HNAGHMKIPMKKBB-UHFFFAOYSA-N 0.000 description 4
- VTHRQKSLPFJQHN-UHFFFAOYSA-N 3-[2-(2-cyanoethoxy)ethoxy]propanenitrile Chemical compound N#CCCOCCOCCC#N VTHRQKSLPFJQHN-UHFFFAOYSA-N 0.000 description 4
- 229920000049 Carbon (fiber) Polymers 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 4
- JGFBQFKZKSSODQ-UHFFFAOYSA-N Isothiocyanatocyclopropane Chemical compound S=C=NC1CC1 JGFBQFKZKSSODQ-UHFFFAOYSA-N 0.000 description 4
- RJUFJBKOKNCXHH-UHFFFAOYSA-N Methyl propionate Chemical compound CCC(=O)OC RJUFJBKOKNCXHH-UHFFFAOYSA-N 0.000 description 4
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 4
- 239000006230 acetylene black Substances 0.000 description 4
- OBNCKNCVKJNDBV-UHFFFAOYSA-N butanoic acid ethyl ester Natural products CCCC(=O)OCC OBNCKNCVKJNDBV-UHFFFAOYSA-N 0.000 description 4
- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 description 4
- 239000004917 carbon fiber Substances 0.000 description 4
- 239000002041 carbon nanotube Substances 0.000 description 4
- 229910021393 carbon nanotube Inorganic materials 0.000 description 4
- 210000004027 cell Anatomy 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- 239000011889 copper foil Substances 0.000 description 4
- 125000004122 cyclic group Chemical group 0.000 description 4
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 4
- 229910021389 graphene Inorganic materials 0.000 description 4
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 description 4
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 4
- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 4
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 description 4
- 229910013872 LiPF Inorganic materials 0.000 description 3
- 101150058243 Lipf gene Proteins 0.000 description 3
- 239000004698 Polyethylene Substances 0.000 description 3
- 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 3
- GNTXTNSKHHBKIB-UHFFFAOYSA-N [O-2].[Ti+4].[Zr+4].[La+3].[Li+].[O-2].[O-2].[O-2].[O-2].[O-2] Chemical compound [O-2].[Ti+4].[Zr+4].[La+3].[Li+].[O-2].[O-2].[O-2].[O-2].[O-2] GNTXTNSKHHBKIB-UHFFFAOYSA-N 0.000 description 3
- 229910052782 aluminium Inorganic materials 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical group [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 3
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 3
- JXGGISJJMPYXGJ-UHFFFAOYSA-N lithium;oxido(oxo)iron Chemical compound [Li+].[O-][Fe]=O JXGGISJJMPYXGJ-UHFFFAOYSA-N 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 description 2
- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 description 2
- FALRKNHUBBKYCC-UHFFFAOYSA-N 2-(chloromethyl)pyridine-3-carbonitrile Chemical compound ClCC1=NC=CC=C1C#N FALRKNHUBBKYCC-UHFFFAOYSA-N 0.000 description 2
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000003490 calendering Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000004146 energy storage Methods 0.000 description 2
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 238000009776 industrial production Methods 0.000 description 2
- 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 2
- 229910003002 lithium salt Inorganic materials 0.000 description 2
- 159000000002 lithium salts Chemical class 0.000 description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 2
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 description 2
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229940017219 methyl propionate Drugs 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- 238000004806 packaging method and process Methods 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 2
- 239000010452 phosphate Substances 0.000 description 2
- 238000001556 precipitation Methods 0.000 description 2
- 238000004886 process control Methods 0.000 description 2
- 229940090181 propyl acetate Drugs 0.000 description 2
- MCSINKKTEDDPNK-UHFFFAOYSA-N propyl propionate Chemical compound CCCOC(=O)CC MCSINKKTEDDPNK-UHFFFAOYSA-N 0.000 description 2
- 229940014800 succinic anhydride Drugs 0.000 description 2
- 238000001291 vacuum drying Methods 0.000 description 2
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 2
- 238000003466 welding Methods 0.000 description 2
- 238000004804 winding Methods 0.000 description 2
- 208000032953 Device battery issue Diseases 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- VFGGFRZVTZVOBE-UHFFFAOYSA-K aluminum titanium(4+) phosphate Chemical compound [Ti+4].P(=O)([O-])([O-])[O-].[Al+3] VFGGFRZVTZVOBE-UHFFFAOYSA-K 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 239000011268 mixed slurry Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
Classifications
-
- 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
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Landscapes
- Secondary Cells (AREA)
Abstract
The invention provides a non-negative electrode lithium ion battery and a preparation method thereof. The non-negative electrode lithium ion battery comprises a positive electrode and a negative electrode, wherein the positive electrode comprises a positive electrode metal current collector and a positive electrode slurry layer arranged on the surface of the positive electrode metal current collector, and the positive electrode slurry layer contains a positive electrode lithium supplementing agent; the cathode comprises a cathode metal current collector and a solid electrolyte layer arranged on the surface of the cathode metal current collector, wherein the preparation raw materials of the solid electrolyte layer comprise solid electrolyte and a solid electrolyte layer binder. All lithium sources in the battery are provided by the positive electrode, and the negative electrode side does not contain active substances, so that the loss of irreversible lithium can be compensated, and the problems of low coulomb efficiency and short cycle life of the non-negative electrode battery are solved. The invention also provides a preparation method of the cathode-free lithium ion battery.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a non-negative electrode lithium ion battery and a preparation method thereof.
Background
In recent years, due to limited energy density of lithium ion batteries, researchers have begun to attempt to build high specific energy lithium metal batteries using high capacity, low voltage lithium metal cathodes. However, the use of excessive lithium metal cathodes generally results in a significant decrease in battery energy density, while excessive lithium continues to consume electrolyte, forming high-resistance byproducts, leading to battery failure. In addition, serious lithium dendrite problems may induce battery safety problems. The non-negative electrode battery configuration can avoid the generation of excessive lithium, thereby greatly improving the safety and energy density of the battery. The non-negative solid-state lithium battery has wide application prospects in next-generation energy storage systems, particularly mobile energy storage systems, due to the ultra-high energy density, higher safety and longer calendar life.
However, the cathode-free battery suffers from problems of low coulombic efficiency, short cycle life, etc., due to limited lithium source inside the battery and poor reversibility of metallic lithium deposition.
Disclosure of Invention
The present invention aims to solve at least one of the above technical problems in the prior art. Therefore, the invention provides a non-negative electrode lithium ion battery, which comprises a positive electrode and a negative electrode, wherein all lithium sources in the battery are provided by the positive electrode, and the negative electrode side does not contain active substances, so that the loss of irreversible lithium can be compensated, and the problems of low coulomb efficiency and short cycle life of the non-negative electrode battery are improved.
The invention also provides a preparation method of the cathode-free lithium ion battery.
A first aspect of the present invention provides a negative electrode-free lithium ion battery comprising:
the positive electrode comprises a positive electrode metal current collector and a positive electrode slurry layer arranged on the surface of the positive electrode metal current collector, wherein the positive electrode slurry layer contains a positive electrode lithium supplementing agent;
the negative electrode comprises a negative electrode metal current collector and a solid electrolyte layer arranged on the surface of the negative electrode metal current collector, wherein the solid electrolyte layer contains solid electrolyte and a solid electrolyte layer binder.
The invention relates to one of the technical schemes of a non-negative lithium ion battery, which has at least the following beneficial effects:
in the non-negative electrode lithium ion battery, the positive electrode comprises the positive electrode metal current collector and the positive electrode slurry layer arranged on the surface of the positive electrode metal current collector, and the positive electrode slurry layer contains the positive electrode lithium supplementing agent, so that the loss of lithium ions in the reaction of the negative electrode solid electrolyte can be compensated. The negative electrode comprises a negative electrode metal current collector and a solid electrolyte layer arranged on the surface of the negative electrode metal current collector, wherein the solid electrolyte layer contains solid electrolyte and a solid electrolyte layer binder, the solid electrolyte has electrophilic property, can induce lithium ion deposition to be uniform, reduces generation of lithium dendrite, and has a more stable structure when the solid electrolyte on the negative electrode current collector is matched with a positive electrode lithium supplementing agent, and the structure of the positive electrode material is more stable, so that the long cycle performance of the non-negative electrode battery is synergistically improved.
According to some embodiments of the invention, the positive electrode slurry layer further contains a positive electrode active material, a conductive agent, a positive electrode slurry layer binder, and a solvent.
According to some embodiments of the invention, the positive electrode active material includes at least one of lithium cobaltate, lithium manganate, and lithium iron phosphate.
According to some embodiments of the invention, the positive electrode active material comprises a ternary material.
According to some embodiments of the invention, the positive electrode active material is added to the positive electrode slurry layer in an amount of 80wt% to 99wt%.
According to some embodiments of the invention, the positive electrode lithium supplementing agent comprises Li 5 FeO 4 、Li 2 NiO 2 、Li 2 O、Li 6 CoO 4 With Li 2 CuO 2 At least one of them.
According to some embodiments of the invention, the positive electrode lithium supplementing agent is added to the positive electrode slurry layer in an amount of 0.1wt% to 5wt%.
According to some embodiments of the invention, in the positive electrode slurry layer, the conductive agent includes at least one of acetylene black, graphene, carbon fiber, and carbon nanotube.
According to some embodiments of the invention, the conductive agent is added to the positive electrode slurry layer in an amount of 0.1wt% to 3wt%.
According to some embodiments of the invention, in the positive electrode slurry layer, the positive electrode slurry layer binder includes polyvinylidene fluoride.
According to some embodiments of the invention, the positive electrode slurry layer binder is added to the positive electrode slurry layer in an amount of 0.1wt% to 2wt%.
According to some embodiments of the invention, in the positive electrode slurry layer, the solvent includes N-methyl-2-pyrrolidone.
According to some embodiments of the invention, the solid electrolyte layer binder comprises at least one of polyvinyl alcohol, polyvinylidene fluoride, and polyethylene oxide.
In the solid electrolyte layer binder, taking polyvinyl alcohol as an example, OH functional groups on the surface of the polyvinyl alcohol can be combined with Li + The C-O-Li bond is formed by reaction to conduct ions, so that lithium ions can be uniformly deposited on the surface of the pole piece, lithium dendrites are reduced, the stability and the rate capability of the battery in the circulation process are improved, and the energy density of the battery can be improved.
According to some embodiments of the invention, the solid electrolyte layer binder is added to the solid electrolyte layer in an amount of 0.1wt% to 3wt%.
When the addition amount of the solid electrolyte layer binder in the solid electrolyte layer is 0.1-3wt%, the solid electrolyte can better act with the solid electrolyte layer binder, so that lithium ions are uniformly deposited on the surface of the pole piece, lithium dendrites are reduced, and the battery performance is improved; beyond the range, the coating effect of the solid electrolyte on the surface of the copper foil is poor, the deposition of lithium ions on the surface of the pole piece is uneven, the lithium precipitation risk is increased, and the safety risk of the battery is increased.
According to some embodiments of the invention, in the negative electrode, the solid electrolyte layer further contains a conductive agent and a solvent.
According to some embodiments of the invention, the solid electrolyte comprisesLithium aluminum titanium phosphate, lithium lanthanum zirconium oxide, lithium lanthanum zirconium titanium oxide, lithium aluminum germanium phosphate, lithium lanthanum titanium oxide and Li 10 GeP 2 S 12 At least one of them.
According to some embodiments of the invention, the solid electrolyte is added to the preparation raw material of the solid electrolyte layer in an amount of 80wt% to 99wt%.
According to some embodiments of the invention, the solid electrolyte is added to the solid electrolyte layer in an amount of 90wt% to 97wt%.
If the content of the solid electrolyte is too small, lithium ions on the positive electrode side are precipitated on the negative electrode side.
According to some embodiments of the invention, in the solid electrolyte layer, the conductive agent includes at least one of acetylene black, graphene, carbon fiber, and carbon nanotube.
According to some embodiments of the invention, the conductive agent is added to the solid electrolyte layer in an amount of 0.1wt% to 3wt%.
According to some embodiments of the invention, the solid electrolyte layer binder has an alcoholysis degree of 75% to 85%.
The alcoholysis degree of the solid electrolyte layer binder is 75-85%, and within the range, the binding property can be ensured, and proper OH functional groups can be combined with Li + The reaction forms a C-O-Li bond to conduct ions, so that lithium ions can be more uniformly deposited on the surface of the pole piece. If too high, the solubility of the adhesive is low, and if too low, the cohesive force itself is too small, and the adhesive strength is lowered.
According to some embodiments of the invention, in the solid electrolyte layer, the solvent comprises N-methyl-2-pyrrolidone.
The second aspect of the invention provides a method for preparing the non-negative electrode lithium ion battery, wherein a diaphragm, the positive electrode and the negative electrode are wound to obtain a bare cell, and the bare cell is packaged after electrolyte is injected to obtain the non-negative electrode lithium ion battery.
The invention relates to a technical scheme in a preparation method of a non-negative electrode lithium ion battery, which at least has the following beneficial effects:
the preparation of the cathode-free lithium ion battery does not need special equipment and complicated process control, the reaction condition is not harsh, the raw materials are easy to obtain, the production cost is low, and the industrial production is easy.
According to some embodiments of the invention, the separator may be a conventional PE-based separator.
According to some embodiments of the invention, the separator has a thickness of 7 μm to 10 μm.
According to some embodiments of the invention, the electrolyte may be a conventional electrolyte, specifically including a lithium salt including lithium hexafluorophosphate (LiPF 6 ) Lithium difluorophosphate (LiPF) 2 O 2 ) Lithium difluorooxalato borate (LiODFB), lithium tetrafluoroborate (LiBF) 4 ) At least one of lithium difluorobis (oxalato) phosphate (LiDFBOP), lithium bis (trifluoromethylsulfonyl) imide (LiTFSI), or lithium bis (fluorosulfonyl) imide (LiFSI).
The organic solvent includes at least one of Ethylene Carbonate (EC), propylene Carbonate (PC), ethylmethyl carbonate (EMC), diethyl carbonate (DEC), ethyl Propionate (EP), propyl Propionate (PP), ethyl Acetate (EA) or gamma-butyrolactone (GBL), methyl Formate (MF), methyl Acetate (MA), ethyl Acetate (EA), propyl acetate (EP), n-Propyl Propionate (PP), methyl propionate (MP, CAS: 554-12-1), methyl Butyrate (MB) and Ethyl Butyrate (EB).
The additive is at least one of ethylene carbonate (VC), 1, 3-Propane Sultone (PS), vinyl sulfate (DTD), maleic anhydride, succinic anhydride, succinonitrile (SN), adiponitrile (ADN), ethylene glycol bis (propionitrile) ether (EGBE) or Hexanetrinitrile (HTCN).
Detailed Description
The following are specific embodiments of the present invention, and the technical solutions of the present invention will be further described with reference to the embodiments, but the present invention is not limited to these embodiments.
In some embodiments of the invention, the invention provides a non-negative lithium ion battery comprising:
the positive electrode comprises a positive electrode metal current collector and a positive electrode slurry layer arranged on the surface of the positive electrode metal current collector, wherein the positive electrode slurry layer contains a positive electrode lithium supplementing agent;
the negative electrode comprises a negative electrode metal current collector and a solid electrolyte layer arranged on the surface of the negative electrode metal current collector, wherein the solid electrolyte layer contains solid electrolyte and a solid electrolyte layer binder.
It can be understood that in the non-negative electrode lithium ion battery, the positive electrode comprises the positive electrode metal current collector and the positive electrode slurry layer arranged on the surface of the positive electrode metal current collector, and the positive electrode slurry layer contains the positive electrode lithium supplementing agent, so that the loss of lithium ions reacted by the negative electrode solid electrolyte can be compensated. The negative electrode comprises a negative electrode metal current collector and a solid electrolyte layer arranged on the surface of the negative electrode metal current collector, wherein the solid electrolyte layer contains solid electrolyte and a solid electrolyte layer binder, the solid electrolyte has electrophilic property, can induce lithium ion deposition to be uniform, reduces generation of lithium dendrite, and has a more stable structure when the solid electrolyte on the negative electrode current collector is matched with a positive electrode lithium supplementing agent, and the structure of the positive electrode material is more stable, so that the long cycle performance of the non-negative electrode is synergistically improved.
In order to further improve the uniformity of deposition of lithium ions on the surface of the solid electrolyte and reduce the generation of lithium dendrites, the binding agent containing OH functional groups of the solid electrolyte layer can be mixed with Li + The C-O-Li bond is formed by reaction to conduct ions, so that lithium ions can be uniformly deposited on the surface of the pole piece, lithium dendrites are reduced, the stability and the rate capability of the battery in the circulation process are improved, and the energy density of the battery can be improved.
In some embodiments of the present invention, the positive electrode slurry layer further contains a positive electrode active material, a conductive agent, a positive electrode slurry layer binder, and a solvent.
In some embodiments of the present invention, the positive electrode active material includes at least one of lithium cobaltate, lithium manganate, and lithium iron phosphate.
In some embodiments of the invention, the positive electrode active material comprises a ternary material.
In some embodiments of the present invention, the positive electrode active material is added to the positive electrode slurry layer in an amount of 80wt% to 99wt%.
In some embodiments of the invention, the positive electrode lithium supplement packageInclude Li 5 FeO 4 、Li 2 NiO 2 、Li 2 O、Li 6 CoO 4 With Li 2 CuO 2 At least one of them.
In some embodiments of the present invention, the positive electrode lithium supplement is added to the positive electrode slurry layer in an amount of 0.1wt% to 5wt%.
In some embodiments of the present invention, in the positive electrode slurry layer, the conductive agent includes at least one of acetylene black, graphene, carbon fiber, and carbon nanotube.
In some embodiments of the present invention, the conductive agent is added to the positive electrode slurry layer in an amount of 0.1wt% to 3wt%.
In some embodiments of the invention, the positive electrode slurry layer binder comprises polyvinylidene fluoride.
In some embodiments of the present invention, the positive electrode slurry layer binder is added to the positive electrode slurry layer in an amount of 0.1wt% to 2wt%.
In some embodiments of the invention, the solvent comprises N-methyl-2-pyrrolidone in the positive electrode slurry layer.
In some embodiments of the invention, the solid electrolyte layer binder comprises at least one of polyvinyl alcohol, polyvinylidene fluoride, and polyethylene oxide.
It will be appreciated that, taking polyvinyl alcohol as an example, the OH functional groups on the surface of the polyvinyl alcohol will be compatible with Li + The C-O-Li bond is formed by reaction to conduct ions, so that lithium ions can be uniformly deposited on the surface of the pole piece, lithium dendrites are reduced, the stability and the rate capability of the battery in the circulation process are improved, and the energy density of the battery can be improved.
In some embodiments of the present invention, the solid electrolyte layer binder is added to the solid electrolyte layer in an amount of 0.1wt% to 3wt%.
When the addition amount of the solid electrolyte layer binder in the solid electrolyte layer is 0.1-3wt%, the solid electrolyte can better act with the solid electrolyte layer binder, so that lithium ions are uniformly deposited on the surface of the pole piece, lithium dendrites are reduced, and the battery performance is improved; beyond the range, the coating effect of the solid electrolyte on the surface of the copper foil is poor, the deposition of lithium ions on the surface of the pole piece is uneven, the lithium precipitation risk is increased, and the safety risk of the battery is increased.
In some embodiments of the invention, the solid electrolyte layer further comprises a conductive agent and a solvent in the negative electrode.
In some embodiments of the invention, the solid state electrolyte comprises lithium aluminum titanium phosphate, lithium lanthanum zirconium oxide, lithium lanthanum zirconium titanium oxide, lithium aluminum germanium phosphate, lithium lanthanum titanium oxide, and Li 10 GeP 2 S 12 At least one of them.
In some embodiments of the present invention, the solid electrolyte is added to the preparation raw material of the solid electrolyte layer in an amount of 80wt% to 99wt%.
In some embodiments of the present invention, the solid electrolyte is added to the solid electrolyte layer in an amount of 90wt% to 97wt%.
If the content of the solid electrolyte is too small, lithium ions on the positive electrode side are precipitated on the negative electrode side.
In some embodiments of the present invention, the conductive agent includes at least one of acetylene black, graphene, carbon fiber, and carbon nanotube in the solid electrolyte layer.
In some embodiments of the present invention, the conductive agent is added to the solid electrolyte layer in an amount of 0.1wt% to 3wt%.
In some embodiments of the invention, the solid electrolyte layer binder has an alcoholysis degree of 75% to 85%.
The alcoholysis degree of the solid electrolyte layer binder is 75-85%, and within the range, the binding property can be ensured, and proper OH functional groups can be combined with Li + The reaction forms a C-O-Li bond to conduct ions, so that lithium ions can be more uniformly deposited on the surface of the pole piece. If too high, the solubility of the adhesive is low, and if too low, the cohesive force itself is too small, and the adhesive strength is lowered.
In some embodiments of the invention, the solvent comprises N-methyl-2-pyrrolidone in the solid state electrolyte layer.
In other embodiments of the present invention, the present invention provides a method for preparing a lithium ion battery without negative electrode, winding a separator with a positive electrode and a negative electrode to obtain a bare cell, injecting an electrolyte, and packaging to obtain the lithium ion battery without negative electrode of the present invention.
It can be understood that the preparation of the cathode-free lithium ion battery does not need special equipment and complex process control, the reaction condition is not harsh, the raw materials are easy to obtain, the production cost is low, and the industrial production is easy.
In some embodiments of the invention, the separator may be a conventional PE-based separator.
In some embodiments of the invention, the thickness of the membrane is 7 μm to 10 μm.
In some embodiments of the invention, the electrolyte may be a conventional electrolyte, specifically including lithium salts including lithium hexafluorophosphate (LiPF), and organic solvents, additives 6 ) Lithium difluorophosphate (LiPF) 2 O 2 ) Lithium difluorooxalato borate (LiODFB), lithium tetrafluoroborate (LiBF) 4 ) At least one of lithium difluorobis (oxalato) phosphate (LiDFBOP), lithium bis (trifluoromethylsulfonyl) imide (LiTFSI), or lithium bis (fluorosulfonyl) imide (LiFSI).
In some embodiments of the invention, the solvent includes at least one of Ethylene Carbonate (EC), propylene Carbonate (PC), ethylmethyl carbonate (EMC), diethyl carbonate (DEC), ethyl Propionate (EP), propyl Propionate (PP), ethyl Acetate (EA) or gamma-butyrolactone (GBL), methyl Formate (MF), methyl Acetate (MA), ethyl Acetate (EA), propyl acetate (EP), n-Propyl Propionate (PP), methyl propionate (MP, CAS: 554-12-1), methyl Butyrate (MB), and Ethyl Butyrate (EB).
In some embodiments of the invention, the additive is at least one of ethylene carbonate (VC), 1, 3-Propane Sultone (PS), vinyl sulfate (DTD), maleic anhydride, succinic anhydride, succinonitrile (SN), adiponitrile (ADN), ethylene glycol bis (propionitrile) ether (EGBE), or Hexanedinitrile (HTCN).
The technical solution of the present invention will be better understood by combining the following specific embodiments.
Example 1
The embodiment prepares a cathode-free lithium ion battery, which comprises:
the positive electrode comprises a positive electrode metal current collector and a positive electrode slurry layer arranged on the surface of the positive electrode metal current collector, wherein the positive electrode slurry layer contains a positive electrode lithium supplementing agent;
the negative electrode comprises a negative electrode metal current collector and a solid electrolyte layer arranged on the surface of the negative electrode metal current collector, wherein the solid electrolyte layer contains solid electrolyte and a solid electrolyte layer binder polyvinyl alcohol.
In the positive electrode:
the positive electrode slurry layer contains a positive electrode active material, a positive electrode lithium supplementing agent, a conductive agent, a binder and a solvent.
The positive electrode active material is lithium cobalt oxide LCO.
The addition amount of the lithium cobalt oxide LCO in the preparation raw material of the positive electrode slurry layer is 95 weight percent.
The positive electrode lithium supplementing agent is lithium-rich lithium ferrite LFO.
The addition amount of the lithium-rich lithium ferrite LFO in the preparation raw material of the positive electrode slurry layer is 1.5 weight percent.
The conductive agent is conductive carbon black.
The addition amount of the conductive carbon black in the preparation raw material of the positive electrode slurry layer was 2wt%.
The binder is polyvinylidene fluoride.
The addition amount of polyvinylidene fluoride in the preparation raw material of the positive electrode slurry layer is 1.5 weight percent.
The solvent is N-methyl-2-pyrrolidone.
The positive metal current collector is aluminum foil.
Mixing positive active material lithium cobalt oxide LCO, positive lithium supplementing agent lithium ferrite LFO, conductive carbon black and adhesive polyvinylidene fluoride, dispersing in N-methyl-2-pyrrolidone to obtain positive electrode slurry, uniformly coating the positive electrode slurry on two sides of an aluminum foil, drying, calendaring and vacuum drying, and welding an aluminum tab by an ultrasonic welder to obtain the positive electrode.
In the negative electrode:
the solid electrolyte is LATP.
The addition amount of LATP in the preparation raw material of the solid electrolyte layer was 97wt%.
The solid electrolyte layer binder is polyvinyl alcohol, and the alcoholysis degree is 80%.
The amount of polyvinyl alcohol added to the solid electrolyte layer was 1.5wt%.
The solid electrolyte layer also contains a conductive agent and a solvent. The conductive agent is conductive carbon black.
The addition amount of the conductive carbon black in the preparation raw material of the solid electrolyte layer was 1.5wt%.
The solvent is N-methyl-2-pyrrolidone.
The negative metal current collector is copper foil.
Mixing the solid electrolyte LATP with polyvinyl alcohol and a conductive agent to obtain uniform mixed slurry, uniformly coating the slurry on two sides of a copper foil, drying, calendaring and vacuum drying, and welding a nickel tab by an ultrasonic welder to obtain the negative electrode.
The preparation method of the cathode-free lithium ion battery comprises the following steps:
and winding the diaphragm, the anode and the cathode to obtain a bare cell, injecting electrolyte, and packaging to obtain the cathode-free lithium ion battery.
The separator is a conventional PE-based separator.
The thickness of the separator was 7 μm.
The electrolyte is lithium hexafluorophosphate electrolyte.
Example 2
This example produced a negative-electrode-free lithium ion battery, differing from example 1 in that the solid electrolyte was Lithium Lanthanum Zirconium Oxide (LLZO).
Example 3
This example produced a negative-electrode-free lithium ion battery, differing from example 1 in that the solid electrolyte was Lithium Lanthanum Zirconium Titanium Oxide (LLZTO).
Example 4
This example produced a negative electrode-free lithium ion battery, differing from example 1 in that the solid state electrolyte was lithium aluminum germanium phosphate (LGPS).
Example 5
This example produced a negative electrode-free lithium ion battery, differing from example 1 in that in the negative electrode, the degree of alcoholysis of polyvinyl alcohol was 84%.
Example 6
This comparative example produces a negative electrode-free lithium ion battery, differing from example 1 in that the solid electrolyte layer binder is polyvinylidene fluoride.
Example 7
This example produced a negative electrode-free lithium ion battery, differing from example 6 in that the amount of the solid electrolyte LATP added in the negative electrode was 88wt%.
Comparative example 1
This comparative example produces a negative electrode-free lithium ion battery, differing from example 1 in that the negative electrode has no solid electrolyte layer.
Comparative example 2
This comparative example produces a negative-electrode-free lithium ion battery, differing from example 1 in that the positive electrode slurry layer does not contain a positive electrode lithium-supplementing agent.
Comparative example 3
This comparative example produces a negative electrode-free lithium ion battery, differing from example 6 in that the solid electrolyte layer binder polyvinylidene fluoride was added in an amount of 0.07wt%.
Comparative example 4
This comparative example produced a negative electrode-free lithium ion battery, differing from example 1 in that in the negative electrode, the polyvinyl alcohol had an alcoholysis degree of 95%.
Performance testing
The batteries prepared in examples and comparative examples were tested for cycle performance and battery initial efficiency. Wherein:
and (3) cyclic test: testing at room temperature 25 ℃): the capacity-divided battery was charged to 4.48V (off current is 0.01C) with a constant current and constant voltage of 0.5C, and then discharged to 3.0V with a constant current of 0.5C.
Cyclic capacity retention (%) = (nth cyclic discharge capacity/1 st cyclic discharge capacity).
Battery first efficiency (%) =capacity-divided discharge capacity/(capacity-divided charge capacity+formation charge capacity) ×100%.
The results are shown in Table 1.
TABLE 1
The results in table 1 show that the lithium-ion battery without the negative electrode provided by the invention can effectively compensate the consumption of lithium ions by the reaction of the solid electrolyte LATP at the negative electrode side under low voltage by adding the lithium supplementing agent at the positive electrode side, the first-week coulomb efficiency of the battery is improved, the solid electrolyte on the surface of the metal current collector of the negative electrode can induce uniform deposition of lithium ions, the generation of lithium dendrites is reduced, the structure of the positive electrode material is more stable when the solid electrolyte on the current collector of the negative electrode is matched with the lithium supplementing agent of the positive electrode, and the long-cycle performance of the negative electrode without the negative electrode is improved by the solid electrolyte on the current collector of the negative electrode.
When the solid electrolyte layer binder is adopted, the polyvinyl alcohol can enable lithium ions to be deposited on the surface of the pole piece more uniformly, reduce lithium dendrites and further improve the stability and the rate capability of the battery in the circulation process.
The present invention has been described in detail with reference to the embodiments, but the present invention is not limited to the embodiments, and various changes can be made within the knowledge of those skilled in the art without departing from the spirit of the present invention.
Claims (10)
1. A negative electrode-less lithium ion battery, comprising:
the positive electrode comprises a positive electrode metal current collector and a positive electrode slurry layer arranged on the surface of the positive electrode metal current collector, wherein the positive electrode slurry layer contains a positive electrode lithium supplementing agent;
the negative electrode comprises a negative electrode metal current collector and a solid electrolyte layer arranged on the surface of the negative electrode metal current collector, wherein the solid electrolyte layer contains solid electrolyte and a solid electrolyte layer binder.
2. The negative electrode-less lithium ion battery of claim 1, wherein the positive electrode slurry layer further comprises a positive electrode active material, a conductive agent, a positive electrode slurry layer binder, and a solvent.
3. The negative electrode-less lithium ion battery of claim 2, wherein the positive electrode active material comprises at least one of lithium cobaltate, lithium manganate, and lithium iron phosphate.
4. The negative electrode-free lithium ion battery according to claim 2, wherein the additive amount of the positive electrode active material in the preparation raw material of the positive electrode slurry layer is 90wt% to 97wt%.
5. The non-negative electrode lithium ion battery of claim 1 or 2, wherein the positive electrode lithium supplement comprises Li 5 FeO 4 、Li 2 NiO 2 、Li 2 O、Li 6 CoO 4 With Li 2 CuO 2 At least one of them.
6. The non-negative electrode lithium ion battery according to claim 1 or 2, wherein the addition amount of the positive electrode lithium supplementing agent in the preparation raw material of the positive electrode slurry layer is 0.1wt% to 5wt%.
7. The negative electrode-less lithium ion battery of claim 1, wherein the solid state electrolyte comprises titanium aluminum lithium phosphate, lithium lanthanum zirconium oxygen, lithium lanthanum zirconium titanium oxygen, aluminum germanium lithium phosphate, lithium lanthanum titanium oxygen, and Li 10 GeP 2 S 12 At least one of (a) and (b); and/or the addition amount of the solid electrolyte in the preparation raw materials of the solid electrolyte layer is 80-99 wt%.
8. The negative electrode-less lithium ion battery of claim 1, wherein the solid electrolyte layer binder comprises at least one of polyvinyl alcohol, polyvinylidene fluoride, and polyethylene oxide; and/or the addition amount of the solid electrolyte layer binder in the solid electrolyte layer is 0.1wt% to 3wt%; and/or, the solid electrolyte layer binder has an alcoholysis degree of 75-85%.
9. The negative electrode-less lithium ion battery of claim 1, wherein the solid electrolyte layer binder is polyvinyl alcohol.
10. A method for preparing the non-negative electrode lithium ion battery according to any one of claims 1 to 9, wherein a separator is wound with the positive electrode and the negative electrode to obtain a bare cell, and the bare cell is packaged after electrolyte is injected to obtain the non-negative electrode lithium ion battery.
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