CN116646527A - Cathode plate, lithium ion battery and power utilization device - Google Patents
Cathode plate, lithium ion battery and power utilization device Download PDFInfo
- Publication number
- CN116646527A CN116646527A CN202310923551.4A CN202310923551A CN116646527A CN 116646527 A CN116646527 A CN 116646527A CN 202310923551 A CN202310923551 A CN 202310923551A CN 116646527 A CN116646527 A CN 116646527A
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- active material
- cathode
- ion conductor
- inorganic single
- single ion
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 26
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 26
- 239000000463 material Substances 0.000 claims abstract description 93
- 239000006182 cathode active material Substances 0.000 claims abstract description 83
- 239000010416 ion conductor Substances 0.000 claims abstract description 69
- 239000011248 coating agent Substances 0.000 claims abstract description 47
- 238000000576 coating method Methods 0.000 claims abstract description 47
- 239000011149 active material Substances 0.000 claims abstract description 37
- -1 halogen sulfide Chemical class 0.000 claims description 23
- 229910013716 LiNi Inorganic materials 0.000 claims description 15
- 239000002105 nanoparticle Substances 0.000 claims description 14
- 229910052782 aluminium Inorganic materials 0.000 claims description 11
- 239000002070 nanowire Substances 0.000 claims description 9
- 239000010936 titanium Substances 0.000 claims description 8
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 6
- RJEIKIOYHOOKDL-UHFFFAOYSA-N [Li].[La] Chemical compound [Li].[La] RJEIKIOYHOOKDL-UHFFFAOYSA-N 0.000 claims description 5
- CDRPLTDFKBZLPZ-UHFFFAOYSA-N [S].[Ge].[P].[Li] Chemical compound [S].[Ge].[P].[Li] CDRPLTDFKBZLPZ-UHFFFAOYSA-N 0.000 claims description 5
- 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 5
- 229910052733 gallium Inorganic materials 0.000 claims description 5
- 229910052736 halogen Inorganic materials 0.000 claims description 5
- 229910052721 tungsten Inorganic materials 0.000 claims description 5
- 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
- 239000004020 conductor Substances 0.000 abstract 1
- 230000005611 electricity Effects 0.000 abstract 1
- 239000003792 electrolyte Substances 0.000 description 45
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 33
- 239000000243 solution Substances 0.000 description 31
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 21
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- 229910000664 lithium aluminum titanium phosphates (LATP) Inorganic materials 0.000 description 16
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- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 14
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- 230000005540 biological transmission Effects 0.000 description 7
- 239000003960 organic solvent Substances 0.000 description 7
- YMWUJEATGCHHMB-UHFFFAOYSA-N Dichloromethane Chemical compound ClCCl YMWUJEATGCHHMB-UHFFFAOYSA-N 0.000 description 6
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 6
- 239000006185 dispersion Substances 0.000 description 6
- HEDRZPFGACZZDS-UHFFFAOYSA-N Chloroform Chemical compound ClC(Cl)Cl HEDRZPFGACZZDS-UHFFFAOYSA-N 0.000 description 4
- 229910020717 Li0.33La0.56TiO3 Inorganic materials 0.000 description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- 230000037427 ion transport Effects 0.000 description 4
- VZGDMQKNWNREIO-UHFFFAOYSA-N tetrachloromethane Chemical compound ClC(Cl)(Cl)Cl VZGDMQKNWNREIO-UHFFFAOYSA-N 0.000 description 4
- VXUYXOFXAQZZMF-UHFFFAOYSA-N titanium(IV) isopropoxide Chemical compound CC(C)O[Ti](OC(C)C)(OC(C)C)OC(C)C VXUYXOFXAQZZMF-UHFFFAOYSA-N 0.000 description 4
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical compound NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 description 3
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- VYMPLPIFKRHAAC-UHFFFAOYSA-N 1,2-ethanedithiol Chemical compound SCCS VYMPLPIFKRHAAC-UHFFFAOYSA-N 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 2
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 description 2
- 229910018091 Li 2 S Inorganic materials 0.000 description 2
- 229910020719 Li0.33 La0.56 Inorganic materials 0.000 description 2
- 229910013553 LiNO Inorganic materials 0.000 description 2
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 2
- 239000004793 Polystyrene Substances 0.000 description 2
- 235000011114 ammonium hydroxide Nutrition 0.000 description 2
- 239000010406 cathode material Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- YBMRDBCBODYGJE-UHFFFAOYSA-N germanium dioxide Chemical compound O=[Ge]=O YBMRDBCBODYGJE-UHFFFAOYSA-N 0.000 description 2
- 239000007791 liquid phase Substances 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- HAUKUGBTJXWQMF-UHFFFAOYSA-N lithium;propan-2-olate Chemical compound [Li+].CC(C)[O-] HAUKUGBTJXWQMF-UHFFFAOYSA-N 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- 238000000643 oven drying Methods 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 229920002223 polystyrene Polymers 0.000 description 2
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- 150000003839 salts Chemical class 0.000 description 2
- 150000003568 thioethers Chemical class 0.000 description 2
- BNGXYYYYKUGPPF-UHFFFAOYSA-M (3-methylphenyl)methyl-triphenylphosphanium;chloride Chemical compound [Cl-].CC1=CC=CC(C[P+](C=2C=CC=CC=2)(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 BNGXYYYYKUGPPF-UHFFFAOYSA-M 0.000 description 1
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- 229920000663 Hydroxyethyl cellulose Polymers 0.000 description 1
- 239000004354 Hydroxyethyl cellulose Substances 0.000 description 1
- 229910021193 La 2 O 3 Inorganic materials 0.000 description 1
- 229910009511 Li1.5Al0.5Ge1.5(PO4)3 Inorganic materials 0.000 description 1
- CERQOIWHTDAKMF-UHFFFAOYSA-N Methacrylic acid Chemical compound CC(=C)C(O)=O CERQOIWHTDAKMF-UHFFFAOYSA-N 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- 239000005062 Polybutadiene Substances 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 229920002125 Sokalan® Polymers 0.000 description 1
- SOXUFMZTHZXOGC-UHFFFAOYSA-N [Li].[Mn].[Co].[Ni] Chemical compound [Li].[Mn].[Co].[Ni] SOXUFMZTHZXOGC-UHFFFAOYSA-N 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
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- 150000001336 alkenes Chemical class 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
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- 229920005549 butyl rubber Polymers 0.000 description 1
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- 239000002041 carbon nanotube Substances 0.000 description 1
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- 229910021389 graphene Inorganic materials 0.000 description 1
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- 229920003088 hydroxypropyl methyl cellulose Polymers 0.000 description 1
- 235000010979 hydroxypropyl methyl cellulose Nutrition 0.000 description 1
- UFVKGYZPFZQRLF-UHFFFAOYSA-N hydroxypropyl methyl cellulose Chemical compound OC1C(O)C(OC)OC(CO)C1OC1C(O)C(O)C(OC2C(C(O)C(OC3C(C(O)C(O)C(CO)O3)O)C(CO)O2)O)C(CO)O1 UFVKGYZPFZQRLF-UHFFFAOYSA-N 0.000 description 1
- 229920002681 hypalon Polymers 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
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- 229920000126 latex Polymers 0.000 description 1
- 239000004816 latex Substances 0.000 description 1
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 1
- 229910002102 lithium manganese oxide Inorganic materials 0.000 description 1
- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 description 1
- 229910001947 lithium oxide Inorganic materials 0.000 description 1
- GLNWILHOFOBOFD-UHFFFAOYSA-N lithium sulfide Chemical compound [Li+].[Li+].[S-2] GLNWILHOFOBOFD-UHFFFAOYSA-N 0.000 description 1
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 description 1
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 description 1
- 238000001755 magnetron sputter deposition Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000003446 memory effect Effects 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 229920001568 phenolic resin Polymers 0.000 description 1
- 239000005011 phenolic resin Substances 0.000 description 1
- 239000006069 physical mixture Substances 0.000 description 1
- 229920002755 poly(epichlorohydrin) Polymers 0.000 description 1
- 229920002627 poly(phosphazenes) Polymers 0.000 description 1
- 239000004584 polyacrylic acid Substances 0.000 description 1
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- 229920000647 polyepoxide Polymers 0.000 description 1
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Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y40/00—Manufacture or treatment of nanostructures
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The application provides a cathode plate, a lithium ion battery and an electricity utilization device. A cathode sheet comprising: a current collector; and an active material layer disposed on at least one surface of the current collector, the active material layer including a cathode active material and an inorganic single ion conductor material, or the active material layer including a surface coated with an inorganic single ionCathode active material of conductor material, the ionic conductivity of the inorganic single ion conductor material is more than or equal to 3 multiplied by 10 ‑3 S/cm; the coating weight of the active material layer was 24 mg/cm 2 ‑43 mg/cm 2 . The application also provides a lithium ion battery comprising the cathode plate and an electric device comprising the lithium ion battery.
Description
Technical Field
The application relates to the technical field of battery material preparation, in particular to a cathode pole piece and a preparation method thereof.
Background
Among a plurality of battery products, the lithium ion battery has the advantages of light weight, small volume, high working voltage, high energy density, high output power, high charging efficiency, no memory effect, long cycle life and the like, and is closely focused by people, so that the lithium ion battery is widely applied to the fields of mobile phones, notebook computers and the like.
In recent years, as the performance of mobile devices and communication devices is continuously improved, higher requirements are being placed on the energy density, cycle life, high-current output and input performance, and the like of lithium ion batteries. Ultra-high nickel cathode active materials have been widely used in lithium ion batteries. The ultra-high nickel cathode active material has the advantage of higher theoretical reversible capacity (> 200 mAh/g) compared with other cathode materials. In addition, the high-energy density lithium ion battery system also needs thicker electrode pole pieces, but the thicker electrode pole pieces cause the lengthening of the lithium ion transmission distance, so that the ion transmission channel is insufficient, and the dynamics is deteriorated.
Disclosure of Invention
Aiming at the problems in the prior art, the application provides a cathode pole piece and a preparation method thereof. The preparation method of the cathode plate is simple, good in repeatability, low in cost and environment-friendly, and the lithium ion battery adopting the cathode plate has higher dynamic performance and energy density.
In a first aspect, the present application provides a cathode sheet comprising:
a current collector; and
the layer of active material is formed of a layer of active material,
the active material layer is disposed on at least one surface of the current collector,
the active material layer comprises a cathode active material and an inorganic single ion conductor material, or the active material layer comprises a cathode active material coated with the inorganic single ion conductor material on the surface,
the ionic conductivity of the inorganic single-ion conductor material is more than or equal to 3 multiplied by 10 -3 S/cm;
The coating weight of the active material layer was 24 mg/cm 2 -43 mg/cm 2 。
In the application, an inorganic single ion conductor is an inorganic fast ion conductor, and refers to a solid inorganic material with ion conductivity approaching or exceeding that of molten salt.
The ionic conductivity of the inorganic single-ion conductor material is tested according to the following method: the powder of the inorganic single-ion conductor material was pressed into a sheet in a mold under a certain pressure (20 MPa) at 25 ℃ as an electrolyte. And placing electrolyte between the blocking electrodes (the blocking electrodes are formed by magnetron sputtering metal spraying), testing the blocking electrodes through EIS, and calculating according to a formula sigma=d/SR to obtain the ion conductivity sigma of the inorganic single-ion conductor material. Wherein d is the electrolyte thickness; s is the effective contact area of the electrode and the electrolyte; r is the intrinsic resistance of the electrolyte.
The cathode plate is designed as a thick film cathode plate. As used herein, the term "thick film cathode sheet" means that the active material layer has a coating weight of 24-43mg/cm 2 Is provided. The thick film electrode of the present application is capable of providing continuous/multiple ion transport channels by incorporating an inorganic single ion conductor material having high ionic conductivity in the cathode active material.
In some embodiments, the inorganic single ion conductor material comprises lithium lanthanum titanyl (Li 0.33 La 0.56 TiO 3 LLTO), lithium aluminum titanium phosphate (Li) 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 LATP), aluminum germanium phosphateLithium (Li) 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 LAGP), lithium germanium phosphorus sulfur (Li) 10 GeP 2 S 12 LGPS), inverse perovskite material (Li 3 OX), glassy sulfide (yLi) 2 S·(100-y)P 2 S 5 ) And halogen sulfide (Li) 6 PS 5 X) wherein 0 < y < 100, and X is selected from Cl, br or I.
Of the above preferred materials, lithium lanthanum titanyl (Li 0.33 La 0.56 TiO 3 LLTO) is about 3 x 10 -3 S/cm; lithium aluminum titanium phosphate (Li) 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 LATP) of about 3 x 10 -3 S/cm; lithium aluminum germanium phosphate (Li) 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 LAGP) of about 6 x 10 -3 S/cm; lithium germanium phosphorus sulfur (Li) 10 GeP 2 S 12 LGPS) of about 4×10 -3 S/cm); inverse perovskite material (Li 3 OX, wherein x=cl, br or I) has an ionic conductivity of about 4X 10 -3 S/cm; glassy sulfides (yLi) 2 S·(100-y)P 2 S 5 ) Is about 5 x 10 -3 S/cm); halogen sulfide (Li) 6 PS 5 X, wherein X is Cl, br or I) has an ionic conductivity of about 5X 10 -3 S/cm。
The inorganic single ion conductor material according to the present application is suitable for physical mixing with or coating all cathode active materials known in the art. The cathode active materials known in the art include, but are not limited to, liCoO 2 A lithium-nickel-cobalt-manganese compound (abbreviated as NCM), a lithium-nickel-cobalt-aluminum compound (NCA), an olivine structure compound (including lithium iron phosphate, lithium manganese iron phosphate, etc.), a spinel structure compound (including lithium manganese oxide, etc.). The cathode active material may also include a mixture of two or more of the above compounds.
Preferably, in some embodimentsThe cathode active material of the present application may include a material having a chemical formula of LiNi m Co n Mn b O 2 One or more of a ternary material, a doped modified material of the ternary material, a clad modified material of the ternary material, wherein m+n+b=1, and 0.96.ltoreq.m.ltoreq.0.995.
In some embodiments, the glassy sulfide may include 25Li 2 S·75 P 2 S 5 。
In some embodiments, the inorganic single ion conductor material may be doped with Ga, ta, W, or Al, among others. Those skilled in the art will appreciate that the inorganic single ion conductor material may be doped with one or more of Ga, ta, W, al, etc., as long as such doping is expected to further enhance its ionic conductivity.
For example, when the inorganic single ion conductor material LLTO is doped with Ga, its ion conductivity will rise to 3.5×10 -3 。
In some embodiments, the inorganic single ion conductor material is a nanoparticle, preferably a nanoparticle of 20-500nm, more preferably a nanoparticle of 50-200 nm; or the inorganic single ion conductor material is a nanowire, preferably a nanowire having an aspect ratio of 5 to 200, more preferably a nanowire having an aspect ratio of 10 to 50. The adoption of nano-scale particles is more beneficial to lithium ion conduction and improves the dynamic performance of the battery.
In some embodiments, the mass of the inorganic single ion conductor material may be 0.1 to 5%, preferably 0.5 to 5%, of the total mass of the inorganic single ion conductor material and the cathode active material.
For example, when the inorganic single ion conductor material of the present application is LLTO and the cathode active material is LiNi 0.96 Co 0.02 Mn 0.02 O 2 When in use, the LLTO/(LLTO+LiNi) 0.96 Co 0.02 Mn 0.02 O 2 ) The mass ratio of (2) may be 0.1 to 5%, preferably 0.5 to 5%.
In some embodiments, the active material layer comprises a physical mixture of a cathode active material and an inorganic single ion conductor material. In some preferred embodiments, the active material layer includes a cathode active material surface-coated with an inorganic single ion conductor material.
In a second aspect, the present application provides a method of preparing a cathode active material incorporating an inorganic single ion conductor material, the method comprising dispersing a precursor of the inorganic single ion conductor material in an organic solvent and then mixing with the cathode active material to obtain a cathode active material incorporating the inorganic single ion conductor material; the application also provides a method for preparing the cathode active material with the inorganic single-ion conductor material coated on the surface, which is simple to operate, and comprises the steps of dispersing the cathode active material in an organic solvent, mixing the organic solvent with a precursor of the inorganic single-ion conductor material, drying and sintering to obtain the cathode active material with the inorganic single-ion conductor material coated on the surface.
In some embodiments, the organic solvent may be selected from one or more of ethanol, ammonia, ethylenediamine, 1, 2-ethanedithiol, ethylene glycol, methanol, cyclohexane, carbon tetrachloride, chloroform, methylene chloride, dimethylformamide, dimethylacetamide, and N-methylpyrrolidone or a mixture thereof, preferably anhydrous ethanol and N-methylpyrrolidone.
The method for preparing the cathode active material with the inorganic single-ion conductor material coated on the surface comprises the steps of dispersing the cathode active material in a proper organic solvent, mixing the cathode active material with a precursor of the inorganic single-ion conductor material to perform more uniform liquid phase coating, and finally sintering at a proper temperature to obtain the cathode active material with the inorganic single-ion conductor material coated on the surface. The method for preparing the cathode active material coated with the inorganic single-ion conductor material on the surface adopts liquid phase coating and sintering, and can remarkably improve the coating uniformity of the inorganic single-ion conductor material.
In a third aspect, the present application provides a method of preparing a cathode sheet comprising:
dispersing the cathode active material introduced with the inorganic single-ion conductor material or the cathode active material coated with the inorganic single-ion conductor material on the surface, a binder and a conductive agent in an organic solvent to form slurry, coating the slurry on the current collector, and drying to obtain the cathode pole piece.
In some embodiments, the binder may be selected from at least one of the group consisting of: carboxymethyl cellulose, hydroxyethyl cellulose, hydroxypropyl methyl cellulose, polyvinylidene fluoride, polytetrafluoroethylene, polyethylene, polypropylene, polybutadiene, butyl rubber, fluororubber, polyoxyethylene, polyvinyl alcohol, polyacrylic acid and its salts, polyvinylpyrrolidone, polyepichlorohydrin, polyphosphazene, polyacrylonitrile, polystyrene, polyvinylpyridine, chlorosulfonated polyethylene, latex, polyester resin, acryl resin, phenolic resin, epoxy resin, polyurethane, polyolefin ester, copolymer of propylene and olefin having 2 to 8 carbon atoms, (meth) acrylic acid and alkyl (meth) acrylate, polystyrene butadiene copolymer and chlorinated rubber, preferably, the binder is polyvinylidene fluoride.
In some embodiments, the conductive agent may be selected from at least one of the following group: natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, carbon fibers, carbon nanotubes, graphene, mesoporous ordered carbon, activated carbon, metal powder, metal fibers and conductive polymers, preferably the conductive agent is super P.
In some embodiments, the inorganic single ion conductor material-incorporated cathode active material or the inorganic single ion conductor material-coated cathode active material comprises 90 to 98 wt% and/or the conductive agent comprises 1 to 5wt% and/or the binder comprises 1 to 5wt%, based on the total weight of the inorganic single ion conductor material-incorporated cathode active material or the inorganic single ion conductor material-coated cathode active material, the binder and the conductive agent.
In some embodiments, the organic solvent may be selected from one or more of ethanol, ethylene glycol, methanol, cyclohexane, carbon tetrachloride, chloroform, methylene chloride, dimethylformamide, dimethylacetamide and N-methylpyrrolidone or a mixture thereof, preferably anhydrous ethanol and N-methylpyrrolidone.
In a fourth aspect, the present application provides a lithium ion battery comprising a cathode electrode sheet, a separator and an anode electrode sheet according to the first aspect of the present application.
In some embodiments, the dynamic performance of the lithium ion battery will be improved by 1.2 to 1.5 times, and the discharge time of the lithium ion battery can be up to 110-130 seconds.
In some embodiments, the energy density of the lithium ion battery may be as high as 400-500Wh/kg.
In a fifth aspect, the present application provides an electrical device comprising a lithium ion battery according to the fourth aspect of the present application, the lithium ion battery being used as a power source for the electrical device.
In a sixth aspect, the present application provides the use of an active material layer comprising a cathode active material and an inorganic single ion conductor material, or comprising a cathode active material surface coated with an inorganic single ion conductor material, for the preparation of a cathode sheet comprising a current collector and an active material layer coated on at least one surface of the current collector, characterized in that the inorganic single ion conductor material has an ionic conductivity of ≡3X10 -3 S/cm, and the coating weight of the active material layer is 24 mg/cm 2 -43 mg/cm 2 。
In some embodiments, the inorganic single ion conductor material is selected from lithium lanthanum titanyl (Li 0.33 La 0.56 TiO 3 LLTO), lithium aluminum titanium phosphate (Li) 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 LATP), lithium aluminum germanium phosphate (Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 LAGP), lithium germanium phosphorus sulfur (Li) 10 GeP 2 S 12 LGPS), inverse perovskite (Li) 3 OX), glassy sulfide (yLi) 2 S·(100-y)P 2 S 5 ) And halogen sulfide (Li) 6 PS 5 X), wherein X is selected from Cl, br or I.
Of the above preferred materials, lithium lanthanum titanyl (Li 0.33 La 0.56 TiO 3 LLTO) is about 3 x 10 -3 S/cm; lithium aluminum titanium phosphate (Li) 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 LATP) of about 3 x 10 -3 S/cm; lithium aluminum germanium phosphate (Li) 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 LAGP) of about 6 x 10 -3 S/cm; lithium germanium phosphorus sulfur (Li) 10 GeP 2 S 12 LGPS) of about 4×10 -3 S/cm); inverse perovskite type (Li) 3 OX, wherein x=cl, br or I) has an ionic conductivity of about 4X 10 -3 S/cm; glassy sulfides (yLi) 2 S·(100-y)P 2 S 5 ) Is about 5 x 10 -3 S/cm); halogen sulfide (Li) 6 PS 5 X, wherein X is Cl, br or I) has an ionic conductivity of about 5X 10 -3 S/cm。
In some embodiments, the cathode active material of the present application may include a material having the formula LiNi m Co n Mn b O 2 One or more of a ternary material, a doped modified material of the ternary material, a clad modified material of the ternary material, wherein m+n+b=1, and 0.96.ltoreq.m.ltoreq.0.995.
In some embodiments, the glassy sulfide may include 25Li 2 S·75 P 2 S 5 。
In some embodiments, the inorganic single ion conductor material may be doped with Ga, ta, W, or Al, among others. Those skilled in the art will appreciate that the inorganic single ion conductor material may be doped with one or more of Ga, ta, W, al, etc., as long as such doping is expected to further enhance its ionic conductivity.
In some embodiments, the inorganic single ion conductor material is a nanoparticle, preferably a nanoparticle of 20-500nm, more preferably a nanoparticle of 50-200 nm; or the inorganic single ion conductor material is a nanowire, preferably a nanowire having an aspect ratio of 5 to 200, more preferably a nanowire having an aspect ratio of 10 to 50.
In some embodiments, the mass of the inorganic single ion conductor material may be 0.1 to 5%, preferably 0.5 to 5%, of the total mass of the inorganic single ion conductor material and the cathode active material. Within this mass ratio, better kinetic properties and energy density can be achieved at the same time.
The following detailed description of the present application will provide further details in order to make the above-mentioned objects, features and advantages of the present application more comprehensible. In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present application. The present application may be embodied in many other forms than described herein and similarly modified by those skilled in the art without departing from the spirit of the application, whereby the application is not limited to the specific embodiments disclosed below.
In the application, the technical characteristics described in an open mode comprise a closed technical scheme composed of the listed characteristics and also comprise an open technical scheme comprising the listed characteristics.
In the present application, the numerical ranges are referred to as continuous, and include the minimum and maximum values of the ranges, and each value between the minimum and maximum values, unless otherwise specified. Further, when a range refers to an integer, each integer between the minimum and maximum values of the range is included. Further, when multiple range description features or characteristics are provided, the ranges may be combined. In other words, unless otherwise indicated, all ranges disclosed herein are to be understood to include any and all subranges subsumed therein.
The temperature parameter in the present application is not particularly limited, and may be a constant temperature treatment or a treatment within a predetermined temperature range. The constant temperature process allows the temperature to fluctuate within the accuracy of the instrument control.
It should be understood that the terms "upper," "lower," and the like, as used herein, are for illustrative purposes only and are not meant to be the only embodiment.
The inventors have noted that a lithium ion battery in the conventional art includes a cathode tab, which generally includes a cathode current collector and an active material layer disposed on the cathode current collector, the active material layer including an active material, a binder, and a conductive agent. However, with development of technology and popularization and application of batteries, the existing cathode pole piece cannot meet the requirements on battery energy density and higher safety. In the manufacturing process of the cathode plate, a ternary system material is generally selected as the cathode material of the cathode plate, and the ternary system material has high energy density and wide application range. However, the demand for higher energy density lithium ion battery systems for cathodes is that cathode active materials in combination with thick film electrode designs are not possible, but thick electrodes result in longer lithium ion transport distances, resulting in insufficient ion transport channels and poor kinetics.
In order to obtain a battery with higher dynamic performance, the applicant researches find that the main material of the cathode active material of the membrane can be selected to have ion conductivity of more than or equal to 3 multiplied by 10 -3 S/cm of inorganic single ion conductor material. Continuous/multiple ion transport channels are provided for thick film electrodes by incorporating inorganic single ion conductor materials with high ionic conductivity into the cathode active material.
The inorganic single ion conductor introduced by the application has a three-dimensional ion transmission channel and high ion conductivity (more than or equal to 3 multiplied by 10) -3 S/cm), has the capability of rapidly conducting ions. After the inorganic single ion conductor is introduced into the cathode active material, the transmission rate of ions on the surface of the cathode active material particles can be promoted, continuous ion transmission channels are formed between the particles, and a multiple ion transmission path is constructed, so that the problem that the transmission capacity of the ions in the thick film electrode is limited is solved, and the dynamic performance is improved.
In some embodiments, the kinetic performance of a lithium ion battery employing a cathode sheet comprising an active material layer of the present application will be improved by a factor of 1.2 to 1.5, particularly as a lithium ion battery can have a discharge time of up to 110-130 seconds and an energy density of up to 400-500Wh/kg.
The advantages of the embodiments of the present application will be further illustrated in the following examples, which are intended to illustrate the application, not to be limiting.
Detailed Description
Example 1: preparation of cathode electrode sheet with active material layer comprising cathode active material surface-coated with LLTO
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 Adding into 100ml of ethanol solution for uniform dispersion;
b. 86.5mg LiNO of LLTO precursor was sequentially added in stoichiometric ratio 3 、691.4mg LaNO 3 And 961.9mg of titanium isopropoxide are added into the ethanol solution and mixed uniformly;
c. heating the solution to be dried, transferring to a furnace, and heating in an air atmosphere at 500 ℃ for 12 hours to obtain a cathode active material with the surface coated with LLTO;
d. the cathode active material with LLTO coated on the surface, a binder PVDF-1 and a conductive agent Super P conductive carbon black are mixed and dispersed in a solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and a thick cathode plate with the coating weight of 30mg/cm is obtained after drying and cold pressing 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 2: preparation of cathode electrode sheet with active Material layer comprising cathode active Material surface-coated with LATP
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 Adding into 100ml of ethanol solution for uniform dispersion;
b. the precursor of LATP is 419.2mg TiCl in sequence according to the stoichiometric ratio 4 、52mg AlCl 3 、382.2ml H 3 PO 4 And 111.8mg of lithium isopropoxide are added into the ethanol solution and mixed uniformly;
c. heating the solution to be dried, transferring to a furnace, and heating in an air atmosphere at 600 ℃ for 12 hours to obtain a cathode active material with the surface coated with LATP;
d. the cathode active material with LATP coated on the surface, a binder PVDF-1 and a conductive agent Super P conductive carbon black are mixed and dispersed in a solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and a thick cathode plate with the coating weight of 26mg/cm is obtained after drying and cold pressing 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 3: preparation of cathode electrode sheet with active material layer comprising cathode active material surface-coated with LAGP
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.97 Co 0.01 Mn 0.02 O 2 Adding into 100ml ammonia water solution for uniform dispersion;
b. 188.3mg germanium dioxide, 43.2mg lithium hydroxide, 127.8mg aluminum nitrate and 352.8ml H as the precursor of LAGP are added in sequence according to the stoichiometric ratio 3 PO 4 Adding into the ammonia water solution and uniformly mixing;
c. heating the solution to be dried, transferring to a furnace, and heating for 12h at 550 ℃ in an air atmosphere to obtain a cathode active material with the surface coated with LAGP;
d. the obtained cathode active material with LAGP coated on the surface, a binder PVDF-1 and a conductive agent Super P conductive carbon black are mixed and dispersed in a solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and a thick cathode plate with the coating weight of 28mg/cm is obtained after drying and cold pressing 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 4: preparation of cathode electrode sheet with active material layer including LGPS-surface-coated cathode active material
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 Adding 40ml of 1, 2-ethylenediamine and 60ml of 1, 2-ethanedithiol solution, and uniformly dispersing;
b. according to the stoichiometric ratio, 391mg of lithium sulfide and 232.2mg of GeS which are precursors of LGPS are sequentially added 2 And 377.9mg P 2 S 5 Adding into the above solution and mixing well;
c. heating the solution to be dried, transferring to a furnace, and heating at 500 ℃ in an inert atmosphere for 6 hours to obtain a cathode active material with the surface coated with LGPS;
d. the obtained cathode active material with LGPS coated on the surface, a binder PVDF-1 and a conductive agent Super P conductive carbon black are mixed and dispersed in a solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and a thick cathode plate with the coating weight of 33mg/cm is obtained after drying and cold pressing 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 5: with surfaces covered with Li 3 Preparation of cathode electrode sheet from active material layer of cathode active material of OCl
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.98 Co 0.01 Mn 0.01 O 2 Adding into 100ml of ethanol solution for uniform dispersion;
b. according to the stoichiometric ratio, li is sequentially added 3 331mg of lithium hydroxide, 414mg of lithium oxide and 585.1mg of lithium chloride which are precursors of OCl are added into the ethanol solution and uniformly mixed;
c. heating the above solution to oven dry, transferring into furnace, and heating at 400deg.C in inert atmosphere for 8 hr to obtain Li-coated solution 3 Cathode active material of OCl;
d. coating the obtained surface with Li 3 The cathode active material of OCl, the binder PVDF-1 and the conductive agent Super P conductive carbon black are mixed and dispersed in solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and the thick cathode pole piece is obtained after drying and cold pressing, wherein the coating weight of the thick cathode pole piece is 35mg/cm 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 6: coated with 25Li by including surface 2 S·75 P 2 S 5 Preparation of cathode electrode sheet from active material layer of cathode active material
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 Adding into 100ml of ethanol solution for uniform dispersion;
b. according to the stoichiometric ratio, 25Li is sequentially added 2 S·75 P 2 S 5 Is 1.5 mg Li 2 S and 935.5mg P 2 S 5 Adding into the ethanol solution and mixing uniformly;
c. heating the above solution to oven drying, transferring into furnace, and heating at 400deg.C in inert atmosphere for 6 hr to obtain a surface coated with 25Li 2 S·75 P 2 S 5 Is used as a cathode active material;
d. coating the obtained surface with 25Li 2 S·75 P 2 S 5 The cathode active material, the binder PVDF-1 and the conductive agent Super P conductive carbon black are mixed and dispersed in a solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and the thick cathode sheet is obtained after drying and cold pressingThe coating weight of the coating is 38mg/cm 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 7: with surfaces covered with Li 6 PS 5 Preparation of cathode electrode sheet from active material layer of cathode active material of Cl
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 Adding into 100ml of ethylenediamine solution, and dispersing uniformly;
b. according to the stoichiometric ratio, li is sequentially added 6 PS 5 Precursor of Cl 644mg Li 2 S, 237.4mgLiCl and 622.4mgP 2 S 5 Adding into the ethanol solution and mixing uniformly;
c. heating the above solution to oven dry, transferring into furnace, and heating at 550deg.C in inert atmosphere for 10 hr to obtain Li-coated solution 6 PS 5 A cathode active material of Cl;
d. coating the obtained surface with Li 6 PS 5 Cathode active material of ClMixing and dispersing the material, a binder PVDF-1 and a conductive agent Super P conductive carbon black in a mass ratio of 97.0wt% to 1.5wt% in a solvent N-methyl pyrrolidone to form slurry, coating the slurry on a cathode current collector, drying and cold pressing to obtain a thick cathode pole piece, wherein the coating weight is 25mg/cm 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 8: with a coating comprising LLTO (Li 0.33 La 0.56 Ga 0.25 Ti 0.75 O 3 ) Preparation of cathode electrode sheet from active material layer of cathode active material
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 Adding into 100ml of ethanol solution for uniform dispersion;
b. in stoichiometric proportion, 84.2mg LiNO of precursor of LLTO doped with Ga is sequentially added 3 、673.2mg LaNO 3 、236.5mg Ga(NO 3 ) 3 And 702.4mg of titanium isopropoxide added to the ethanolMixing the above materials in solution;
c. heating the above solution to oven drying, transferring to furnace, and heating at 500deg.C in air atmosphere for 12 hr to obtain LLTO (Li) 0.33 La 0.56 Ga 0.25 Ti 0.75 O 3 ) Is used as a cathode active material;
d. coating the obtained LLTO (Li 0.33 La 0.56 Ga 0.25 Ti 0.75 O 3 ) The cathode active material, the binder PVDF-1 and the conductive agent Super P conductive carbon black are mixed and dispersed in a solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and the thick cathode sheet is obtained after drying and cold pressing, wherein the coating weight is 36mg/cm 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Example 9: preparation of cathode electrode sheet with active material layer comprising cathode active material incorporating LATP
419.2mg TiCl of LATP precursor 4 、52mg AlCl 3 、382.2ml H 3 PO 4 And 111.8mg of lithium isopropoxide are added to 100ml of ethanol solution and mixed uniformly, the above solution is heated to dryness, and then transferred to a furnace, and heated in an air atmosphere at 600 ℃ for 12 hours to obtain LATP.
Mixing the LATP with 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 The mixture of the adhesive polyvinylidene fluoride and the conductive agent Super P is mixed and dispersed in the solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and the thick cathode pole piece is obtained after drying and cold pressing, wherein the coating weight of the thick cathode pole piece is 26mg/cm 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Comparative example 1: preparation of cathode electrode sheet with active material layer including cathode active material surface-coated with LLZO
The preparation method comprises the following steps:
a. 100g of cathode active material LiNi 0.96 Co 0.02 Mn 0.02 O 2 Added toUniformly dispersing in 100ml of ethanol solution;
b. LLZO (with ionic conductivity of 1.8X10) -3 S/cm), 141.4mg LiOH, 205.1mg La 2 O 3 And 360.2mg ZrO 2 Adding into the ethanol solution and mixing uniformly;
c. heating the solution to be dried, transferring to a furnace, and heating in an air atmosphere at 500 ℃ for 12 hours to obtain a cathode active material with the surface coated with LLZO;
d. the cathode active material with LLZO coated on the surface, a binder PVDF-1 and a conductive agent Super P conductive carbon black are mixed and dispersed in a solvent N-methyl pyrrolidone according to the mass ratio of 97.0wt percent to 1.5wt percent to form slurry, the slurry is coated on a cathode current collector, and a thick cathode plate with the coating weight of 30mg/cm is obtained after drying and cold pressing 2 。
Optionally, the cathode sheet obtained in the step d and the following cathode sheet, separator and electrolyte are further used for preparing a battery:
negative pole piece: dissolving negative electrode active material graphite, conductive agent Super P conductive carbon black and binder styrene-butadiene rubber (SBR) in solvent deionized water according to the weight ratio of 92:4:4, and uniformly mixing to prepare negative electrode slurry; and uniformly coating the negative electrode slurry on a negative electrode current collector copper foil once or a plurality of times, and drying, cold pressing and cutting to obtain a negative electrode plate.
Isolation film: PE film with ceramic coating.
Electrolyte solution: lithium hexafluorophosphate LiPF6 was used as an electrolyte, the content thereof in the electrolyte was 10%, and a mixture of ec+pc (ethylene carbonate+propylene carbonate) in a volume ratio of 3:7 was used as a solvent.
And forming a bare cell by the positive pole piece, the negative pole piece and the isolating film, insulating and coating the bare cell, then filling the bare cell into an aluminum shell, and welding a top cover to obtain the dry cell. And baking the dry battery core, injecting electrolyte, and performing formation and aging to obtain the hard-shell battery.
Experimental example 1: characterization of kinetic properties of batteries prepared with the cathode Pole pieces of the examples of the application
The batteries (modified group) prepared by the cathode tabs of examples 1 to 9 of the present application and the control battery (battery prepared by the cathode tab of comparative example 1) were discharged at 40% soc with 5C magnification, and the discharge time t was recorded to characterize the kinetic properties, and the results are as follows.
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Claims (14)
1. A cathode sheet comprising:
a current collector; and
the layer of active material is formed of a layer of active material,
the active material layer is disposed on at least one surface of the current collector,
the active material layer comprises a cathode active material and an inorganic single ion conductor material, or the active material layer comprises a cathode active material coated with the inorganic single ion conductor material on the surface,
the ionic conductivity of the inorganic single-ion conductor material is more than or equal to 3 multiplied by 10 -3 S/cm;
The coating weight of the active material layer was 24 mg/cm 2 -43 mg/cm 2 。
2. The cathode sheet of claim 1, wherein the inorganic single ion conductor material comprises at least one of the group consisting of: lithium lanthanum titanyl (Li) 0.33 La 0.56 TiO 3 ) Lithium titanium aluminum phosphate (Li) 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 ) Lithium germanium aluminum phosphate (Li) 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 ) Lithium germanium phosphorus sulfur (Li) 10 GeP 2 S 12 ) Inverse perovskite material (Li 3 OX), glassy sulfide (yLi) 2 S·(100-y)P 2 S 5 ) And halogen sulfide (Li) 6 PS 5 X), wherein 0 < y < 100, X is selected from Cl, br or I.
3. According to claimThe cathode sheet of claim 1, wherein the cathode active material comprises a material having the formula LiNi m Co n Mn b O 2 One or more of a ternary material, a doped modified material of the ternary material, a clad modified material of the ternary material, wherein m+n+b=1, and 0.96.ltoreq.m.ltoreq.0.995.
4. The cathode pole piece of claim 2, wherein the glassy sulfide is 25Li 2 S·75 P 2 S 5 。
5. The cathode sheet according to claim 1, wherein the inorganic single ion conductor material is doped with one or more of Ga, ta, W and Al elements.
6. The cathode sheet according to claim 1, wherein the inorganic single ion conductor material is a nanoparticle; or the inorganic single ion conductor material is a nanowire.
7. The cathode sheet according to claim 1, wherein the inorganic single ion conductor material is a nanoparticle, the nanoparticle being a nanoparticle of 20-500 nm.
8. The cathode sheet according to claim 1, wherein the inorganic single ion conductor material is a nanoparticle, the nanoparticle being a nanoparticle of 50-200 nm.
9. The cathode sheet according to claim 1, wherein the inorganic single ion conductor material is a nanowire having an aspect ratio of 5-200.
10. The cathode sheet according to claim 1, wherein the inorganic single ion conductor material is a nanowire having an aspect ratio of 10-50.
11. The cathode sheet according to claim 1, wherein the mass of the inorganic single ion conductor material is 0.1% -5% of the total mass of the inorganic single ion conductor material and the cathode active material.
12. The cathode sheet according to claim 1, wherein the mass of the inorganic single ion conductor material is 0.5% -5% of the total mass of the inorganic single ion conductor material and the cathode active material.
13. A lithium ion battery comprising the cathode sheet of any one of claims 1-12.
14. An electrical device comprising the lithium ion battery of claim 13.
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