CN113937253A - Simple method for improving positive performance of lithium ion battery - Google Patents
Simple method for improving positive performance of lithium ion battery Download PDFInfo
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- CN113937253A CN113937253A CN202111178165.4A CN202111178165A CN113937253A CN 113937253 A CN113937253 A CN 113937253A CN 202111178165 A CN202111178165 A CN 202111178165A CN 113937253 A CN113937253 A CN 113937253A
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- 238000000034 method Methods 0.000 title claims abstract description 22
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 10
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 10
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 20
- 238000002156 mixing Methods 0.000 claims abstract description 8
- 239000007774 positive electrode material Substances 0.000 claims abstract description 8
- 239000002002 slurry Substances 0.000 claims abstract description 8
- 238000002360 preparation method Methods 0.000 claims abstract description 7
- 239000011572 manganese Substances 0.000 claims description 13
- 239000000463 material Substances 0.000 claims description 12
- 229910052748 manganese Inorganic materials 0.000 claims description 11
- 239000000843 powder Substances 0.000 claims description 11
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 9
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 9
- 229910052744 lithium Inorganic materials 0.000 claims description 9
- 229910000473 manganese(VI) oxide Inorganic materials 0.000 claims description 9
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 claims description 5
- 239000011248 coating agent Substances 0.000 claims description 5
- 238000000576 coating method Methods 0.000 claims description 5
- 239000002033 PVDF binder Substances 0.000 claims description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 4
- 239000002228 NASICON Substances 0.000 claims description 2
- 229910019142 PO4 Inorganic materials 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 2
- 239000011230 binding agent Substances 0.000 claims description 2
- 239000011888 foil Substances 0.000 claims description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 2
- 239000010452 phosphate Substances 0.000 claims description 2
- 239000002904 solvent Substances 0.000 claims description 2
- 239000002223 garnet Substances 0.000 claims 1
- 239000002994 raw material Substances 0.000 claims 1
- 229910052718 tin Inorganic materials 0.000 claims 1
- 239000003792 electrolyte Substances 0.000 abstract description 3
- 239000010405 anode material Substances 0.000 abstract description 2
- 238000007086 side reaction Methods 0.000 abstract description 2
- 229910008026 Li1+x+yAlxTi2-xSiyP3-yO12 Inorganic materials 0.000 description 6
- 229910008043 Li1+x+yAlxTi2−xSiyP3-yO12 Inorganic materials 0.000 description 6
- 229910006188 Li1+x+yAlxTi2−xSiyP3−yO12 Inorganic materials 0.000 description 6
- 239000013543 active substance Substances 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 229910001346 0.5Li2MnO3 Inorganic materials 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000000157 electrochemical-induced impedance spectroscopy Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229910002983 Li2MnO3 Inorganic materials 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000006258 conductive agent Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 238000013467 fragmentation Methods 0.000 description 1
- 238000006062 fragmentation reaction Methods 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 239000011268 mixed slurry Substances 0.000 description 1
- 239000003607 modifier Substances 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 238000004611 spectroscopical analysis Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910006525 α-NaFeO2 Inorganic materials 0.000 description 1
- 229910006596 α−NaFeO2 Inorganic materials 0.000 description 1
Images
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1391—Processes of manufacture of 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
- 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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/366—Composites as layered products
-
- 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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
-
- 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
- H01M4/625—Carbon or graphite
-
- 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 invention discloses a method for improving the performance of a positive active material of a lithium ion battery by simple measures, namely simply and mechanically mixing a solid electrolyte and the positive active material or directly adding the solid electrolyte in the preparation process of slurry, thereby improving the comprehensive electrochemical performance of a positive plate. The invention reduces the contact area of the anode material and the electrolyte, can effectively inhibit surface side reaction, and does not influence the transportation of lithium ions. The invention has the characteristics of low technical requirement, simple operation, low cost, obvious effect and the like.
Description
Technical Field
The invention belongs to the technical field of lithium ion battery anodes, and particularly relates to a method for improving the electrochemical performance of a lithium ion anode plate by adopting simple measures.
Background
Lithium ion batteries have been widely used in a plurality of fields such as digital code, electronic information, traffic, energy storage and the like, and the anode material thereof is the most important factor limiting the performance of the lithium ion battery. The positive electrode material is unstable in the charging and discharging process and is often accompanied by side reactions between the surface of the material and the electrolyte, degradation of the crystal structure of the material, fragmentation of the electrode structure, falling of the active coating and the like. The traditional improvement measures comprise active material bulk phase doping and surface coating, electrolyte component improvement, battery manufacturing process and formation process optimization and the like. On the basis of the finished electrode active material, a simple and effective measure is adopted in the manufacturing process of the electrode plate, and the improvement of the surface chemical stability and the electrochemical performance of the material is obviously meaningful work.
Disclosure of Invention
The invention provides a method which does not change the preparation process route of the existing lithium ion battery, has flexible and adjustable formula and can effectively coat active substances so as to improve the electrochemical performance of a battery anode, and the method comprises the following steps:
(1) adding solid electrolyte in the slurry preparation process, wherein the introduction mode can be that the positive active material is mixed with the solid electrolyte in advance, or the solid electrolyte can be added in the slurry preparation process;
(2) according to the traditional process route, adding a carbon material conductive agent, a binder and a solvent (NMP) for uniform dispersion;
(3) and coating and drying the prepared slurry to prepare the positive electrode slice.
The optimized amount of the solid electrolyte added in the step (1) is 10%.
The positive active substance in the step (1) is a lithium-rich manganese-based positive material, and the molecular formula of the positive active substance is xLi2MnO3·(1-x)LiTMO2(TM is at least one of Ni, Co and Mn), and x is more than or equal to 0.1 and less than or equal to 0.9, and the material has both R3m space group and C2/m space group.
The solid electrolyte in the step (1) is a lithium-substituted NASICON phosphate of which the molecular formula is Li1+x+ yAlxTi2-xSiyP3-yO12Wherein 0 is<x<2,0<y<3。
Compared with the prior art, the method has the advantages that the positive active material modifier is added in the size mixing process, the electrochemical performance of the positive plate is effectively improved, and the method has the characteristics of low technical requirement, simplicity in operation, low cost and the like.
Drawings
FIG. 1 shows xLi used in example 1 of the present invention2MnO3·(1-x)LiTMO2X-ray diffraction Spectroscopy (XRD) of the powder.
Fig. 2 is a Transmission Electron Microscope (TEM) photograph of the solid electrolyte used in example 1 of the present invention.
FIG. 3 shows xLi in example 1 of the present invention2MnO3·(1-x)LiTMO2And solid electrolyte Li1+x+yAlxTi2- xSiyP3-yO12Mixing the powder with xLi2MnO3·(1-x)LiTMO2The first charge-discharge curve of the positive plate prepared from the pure powder.
FIG. 4 shows xLi in example 1 of the present invention2MnO3·(1-x)LiTMO2And solid electrolyte Li1+x+yAlxTi2- xSiyP3-yO12Mixing the powder with xLi2MnO3·(1-x)LiTMO2The relationship between the charge and discharge times and the discharge specific capacity of the positive plate prepared from the pure powder under the current multiplying power of 1C.
FIG. 5 shows xLi in example 1 of the present invention2MnO3·(1-x)LiTMO2And solid electrolyte Li1+x+yAlxTi2- xSiyP3-yO12Mixing the powder with xLi2MnO3·(1-x)LiTMO2The positive plate prepared from pure powder is 105~10-2Electrochemical Impedance Spectroscopy (EIS) in HZ frequency interval under 5mV sinusoidal AC signal disturbance.
Detailed Description
In order to facilitate an understanding of the invention, the invention will be described more fully and in detail below with reference to the accompanying drawings and preferred embodiments, but the scope of the invention is not limited to the specific embodiments below.
Unless otherwise defined, all terms of art used hereinafter have the same meaning as commonly understood by one of ordinary skill in the art. The terminology used herein is for the purpose of describing particular embodiments only and is not intended to limit the scope of the present invention.
Unless otherwise specified, the reagents and materials used in the present invention are commercially available products or products obtained by a known method.
Example 1:
0.5Li2MnO3·0.5LiNi0.13Co0.13Mn0.54O2Powder, solid electrolyte Li1+x+yAlxTi2-xSiyP3- yO12Mixing and grinding acetylene black, CNTs slurry and polyvinylidene fluoride (PVDF) in a dry powder mass ratio of 82:10:2:1:5, and adding N-methyl pyrrolidone (NMP) for size mixing. And coating the mixed slurry on the surface of an aluminum foil, and then drying, cutting and assembling to prepare the CR2032 half-cell.
As can be seen from FIG. 1, the lithium-rich manganese cathode material 0.5Li2MnO3·0.5LiNi0.13Co0.13Mn0.54O2The powder is alpha-NaFeO2Layer-shaped structure with associated Li2MnO3A superlattice structure, and the crystallinity of the material is good; as can be seen from FIG. 2, the solid electrolyte Li1+x+yAlxTi2-xSiyP3-yO12The particle size of the particles is between 10 and 40nm, and the particle size distribution is relatively concentrated; as can be seen from the attached figure 3, the first discharge specific capacity of the lithium-rich manganese mixed with the solid electrolyte is about 260mAh/g, which is improved by about 40mAh/g compared with pure lithium-rich manganese powder; as can be seen from fig. 4, the cycle capacity of the lithium-rich manganese and solid electrolyte mixed electrode plate is obviously higher than that of the pure lithium-rich manganese electrode plate; as can be seen from fig. 5, the impedance of the electrochemical reaction of the lithium-rich manganese and solid electrolyte mixed electrode plate is about 170 Ω, which is significantly lower than about 240 Ω of the pure lithium-rich manganese electrode plate.
Claims (5)
1. A method for improving the electrochemical performance of a positive electrode plate of a lithium ion battery comprises the following steps:
(1) mechanically mixing the positive active material with the solid electrolyte in advance, or adding the solid electrolyte at any stage of slurry preparation;
(2) and (2) preparing the slurry according to the traditional process on the basis of the step (1), and normally coating the slurry on the aluminum foil without adding extra working procedures.
2. The method for improving the electrochemical performance of the positive plate according to claim 1, wherein the solid electrolyte in the step (1) accounts for 5-50% of the whole dry powder raw material of the positive plate.
3. The method for improving the electrochemical performance of the positive plate according to claim 1, wherein the positive active material in the step (1) is a lithium-rich manganese-based positive material or a conventional ternary positive material, and the molecular formulas of the positive active material and the conventional ternary positive material are respectively xLi2MnO3·(1-x)LiTMO2(wherein x is 0.1. ltoreq. x.ltoreq.0.9, and TM is at least one of Ni, Co, and Mn) and LiTMO2(wherein TM is Ni, Co, Mn), the solid electrolyte may be a lithium-substituted NASICON phosphate or garnet-type LimLanZrzO2Garnet type LimLanZrzMtO2(M is one or more of Ti, Pb, Sn and … …, 8<m+n<12,1<z<3,1<z+t<5)。
4. The method for improving the electrochemical performance of the positive electrode sheet according to claim 1, wherein the conventional process in the step (2) is a wet preparation process using N-methylpyrrolidone (NMP) as a solvent and polyvinylidene fluoride (PVDF) as a binder.
5. The method for improving the electrochemical performance of the positive electrode sheet according to claim 1, wherein the step (2) of not adding extra processes is that adding corresponding materials according to design requirements during the material preparation process does not belong to an extra process.
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114784223A (en) * | 2022-04-28 | 2022-07-22 | 广东马车动力科技有限公司 | Positive plate and preparation method and application thereof |
CN114944488A (en) * | 2022-05-23 | 2022-08-26 | 浙江锂威能源科技有限公司 | Preparation method of coated positive electrode material, product and application thereof |
Citations (4)
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CN104937749A (en) * | 2013-01-25 | 2015-09-23 | 丰田自动车株式会社 | Positive electrode for secondary cell, method for manufacturing positive electrode for secondary cell, and whole solid secondary cell |
CN105932225A (en) * | 2016-06-29 | 2016-09-07 | 中国科学院青岛生物能源与过程研究所 | Preparation method of improved room temperature electron ion fast transfer electrode slice for solid-state secondary lithium battery |
CN109638233A (en) * | 2018-10-26 | 2019-04-16 | 国联汽车动力电池研究院有限责任公司 | A kind of solid state ionic conductor and lithium-rich manganese base material combination electrode and lithium ion battery |
CN109860550A (en) * | 2019-01-25 | 2019-06-07 | 浙江衡远新能源科技有限公司 | A kind of preparation method of solid state lithium battery anode composite film |
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2021
- 2021-10-09 CN CN202111178165.4A patent/CN113937253A/en active Pending
Patent Citations (4)
Publication number | Priority date | Publication date | Assignee | Title |
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CN104937749A (en) * | 2013-01-25 | 2015-09-23 | 丰田自动车株式会社 | Positive electrode for secondary cell, method for manufacturing positive electrode for secondary cell, and whole solid secondary cell |
CN105932225A (en) * | 2016-06-29 | 2016-09-07 | 中国科学院青岛生物能源与过程研究所 | Preparation method of improved room temperature electron ion fast transfer electrode slice for solid-state secondary lithium battery |
CN109638233A (en) * | 2018-10-26 | 2019-04-16 | 国联汽车动力电池研究院有限责任公司 | A kind of solid state ionic conductor and lithium-rich manganese base material combination electrode and lithium ion battery |
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Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
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CN114784223A (en) * | 2022-04-28 | 2022-07-22 | 广东马车动力科技有限公司 | Positive plate and preparation method and application thereof |
CN114944488A (en) * | 2022-05-23 | 2022-08-26 | 浙江锂威能源科技有限公司 | Preparation method of coated positive electrode material, product and application thereof |
CN114944488B (en) * | 2022-05-23 | 2024-02-09 | 浙江锂威能源科技有限公司 | Preparation method of coated positive electrode material, product and application thereof |
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