CN113871725B - Non-negative electrode lithium secondary battery - Google Patents
Non-negative electrode lithium secondary battery Download PDFInfo
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- CN113871725B CN113871725B CN202111143905.0A CN202111143905A CN113871725B CN 113871725 B CN113871725 B CN 113871725B CN 202111143905 A CN202111143905 A CN 202111143905A CN 113871725 B CN113871725 B CN 113871725B
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- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 91
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 87
- 239000003792 electrolyte Substances 0.000 claims abstract description 21
- 239000007774 positive electrode material Substances 0.000 claims abstract description 19
- 239000000463 material Substances 0.000 claims abstract description 17
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- 239000002033 PVDF binder Substances 0.000 claims description 21
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- 239000013538 functional additive Substances 0.000 claims description 12
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 11
- 229910010293 ceramic material Inorganic materials 0.000 claims description 11
- -1 propenesulfonic acid lactone Chemical class 0.000 claims description 11
- 239000011149 active material Substances 0.000 claims description 9
- 239000010410 layer Substances 0.000 claims description 9
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 8
- 239000003960 organic solvent Substances 0.000 claims description 8
- 150000003839 salts Chemical class 0.000 claims description 8
- 239000011247 coating layer Substances 0.000 claims description 7
- 150000001875 compounds Chemical class 0.000 claims description 5
- 229910001346 0.5Li2MnO3 Inorganic materials 0.000 claims description 4
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- 229910002983 Li2MnO3 Inorganic materials 0.000 claims description 4
- 229910018434 Mn0.5O2 Inorganic materials 0.000 claims description 4
- 229910019142 PO4 Inorganic materials 0.000 claims description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
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- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 3
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 3
- 125000003275 alpha amino acid group Chemical group 0.000 claims description 3
- GWAOOGWHPITOEY-UHFFFAOYSA-N 1,5,2,4-dioxadithiane 2,2,4,4-tetraoxide Chemical compound O=S1(=O)CS(=O)(=O)OCO1 GWAOOGWHPITOEY-UHFFFAOYSA-N 0.000 claims description 2
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 claims description 2
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 2
- NEILRVQRJBVMSK-UHFFFAOYSA-N B(O)(O)O.C[SiH](C)C.C[SiH](C)C.C[SiH](C)C Chemical compound B(O)(O)O.C[SiH](C)C.C[SiH](C)C.C[SiH](C)C NEILRVQRJBVMSK-UHFFFAOYSA-N 0.000 claims description 2
- 229910019119 CobMcO2 Inorganic materials 0.000 claims description 2
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- 229910052742 iron Inorganic materials 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
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- ZRZFJYHYRSRUQV-UHFFFAOYSA-N phosphoric acid trimethylsilane Chemical compound C[SiH](C)C.C[SiH](C)C.C[SiH](C)C.OP(O)(O)=O ZRZFJYHYRSRUQV-UHFFFAOYSA-N 0.000 claims description 2
- 229920002635 polyurethane Polymers 0.000 claims description 2
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- 229910052721 tungsten Inorganic materials 0.000 claims description 2
- 229910052720 vanadium Inorganic materials 0.000 claims description 2
- 239000011787 zinc oxide Substances 0.000 claims description 2
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 abstract description 10
- 239000011889 copper foil Substances 0.000 abstract description 10
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- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 5
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 5
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- 239000007773 negative electrode material Substances 0.000 description 5
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- HNAGHMKIPMKKBB-UHFFFAOYSA-N 1-benzylpyrrolidine-3-carboxamide Chemical compound C1C(C(=O)N)CCN1CC1=CC=CC=C1 HNAGHMKIPMKKBB-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- JGFBQFKZKSSODQ-UHFFFAOYSA-N Isothiocyanatocyclopropane Chemical compound S=C=NC1CC1 JGFBQFKZKSSODQ-UHFFFAOYSA-N 0.000 description 1
- 229910013716 LiNi Inorganic materials 0.000 description 1
- 229910001290 LiPF6 Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 0.000 description 1
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
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- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
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- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 description 1
- 238000005524 ceramic coating Methods 0.000 description 1
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- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
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- 229910001416 lithium ion Inorganic materials 0.000 description 1
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 description 1
- 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 1
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical group C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
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- 239000011259 mixed solution Substances 0.000 description 1
- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000013585 weight reducing agent Substances 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative 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
-
- 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
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Secondary Cells (AREA)
Abstract
The invention belongs to the field of lithium secondary batteries, and particularly relates to a non-negative electrode lithium secondary battery. The non-negative electrode lithium secondary battery comprises a positive electrode, a negative electrode, a diaphragm and electrolyte, wherein the positive electrode active substance of the positive electrode is a lithium-containing material with the first efficiency lower than 85%. In the invention, the positive electrode adopts a low first-effect lithium-containing material, lithium in the positive electrode material migrates to the surface of a negative electrode copper foil during the first charge, and a lithium layer is formed on the surface of the copper foil, thus completing the lithium plating of the copper foil negative electrode. Because of the low first effect of the positive electrode material, a large amount of irreversible lithium can not migrate back to the surface of the positive electrode, but still can be on the negative electrode side, so that the negative electrode is supplemented with lithium, and the consumption of reversible active lithium in the cycle process can be compensated by the part of lithium, so that the purposes of improving the coulombic efficiency and the cycle performance in the cycle process are achieved.
Description
Technical Field
The invention belongs to the field of lithium secondary batteries, and particularly relates to a non-negative electrode lithium secondary battery.
Background
With the large-scale application and development of new energy electric automobiles, smart phones and other consumer electronic devices, higher requirements are put on the weight reduction and energy density of lithium batteries. According to the existing liquid lithium ion power battery which is formed by taking ternary and graphite as positive and negative electrode active materials, the weight energy density limit is about 280 Wh/kg. Even if silicon-based alloy is introduced to replace pure graphite as the negative electrode material, the upper limit of the energy density can only reach 300-350Wh/kg.
Metallic lithium is considered to be an ideal negative electrode material due to its extremely high theoretical gram capacity (3860 mAh/g, about 10 times that of graphite) and lower reduction potential (3.045V versus standard hydrogen electrode). And the energy density of the lithium metal secondary battery adopting the metal lithium as the negative electrode can reach more than 400wh/kg, and even is hopeful to exceed 500wh/kg. However, when lithium metal is used as a negative electrode of a battery, since lithium metal has high reactivity as an alkali metal and reacts and explodes with oxygen and water in the air, lithium metal batteries have very severe demands on manufacturing environments, and cannot be manufactured in conventional environments.
The non-negative electrode lithium secondary battery does not use a negative electrode active material, only adopts a negative electrode current collector as a negative electrode, completes negative electrode lithium plating in the first charging process, returns to the positive electrode during discharging, and realizes charge and discharge circulation. The non-negative electrode lithium secondary battery not only greatly improves the capacity density of the battery, but also can avoid inconvenience and potential safety hazard caused by using the metal lithium sheet in the actual production and manufacturing process, reduces the requirement on the production environment and improves the production efficiency.
However, the development of non-negative cells is limited due to the low coulombic efficiency and faster capacity fade during cycling of non-negative cells.
Disclosure of Invention
The invention aims to provide a non-negative electrode lithium secondary battery, which not only avoids the safety risk caused by using a metal lithium sheet in the battery manufacturing process, but also improves the problem of poor circulation of the non-negative electrode battery using the traditional positive electrode material.
In order to achieve the above object, the technical scheme of the non-negative electrode lithium secondary battery of the present invention is as follows:
A non-negative electrode lithium secondary battery comprises a positive electrode, a negative electrode, a diaphragm and electrolyte, wherein the positive electrode active substance of the positive electrode is a lithium-containing material with the first efficiency lower than 85%.
In the invention, the positive electrode adopts a low first-effect lithium-containing material, lithium in the positive electrode material migrates to the surface of a negative electrode copper foil during the first charge, and a lithium layer is formed on the surface of the copper foil, thus completing the lithium plating of the copper foil negative electrode. Because of the low first effect of the positive electrode material, a large amount of irreversible lithium can not migrate back to the surface of the positive electrode, but still can be on the negative electrode side, so that the negative electrode is supplemented with lithium, and the consumption of reversible active lithium in the cycle process can be compensated by the part of lithium, so that the purposes of improving the coulombic efficiency and the cycle performance in the cycle process are achieved.
Preferably, the first efficiency of the positive electrode active material is not higher than 80%. More preferably not less than 60% and not more than 82%.
Further preferably, the lithium-containing material is selected from one or more of compounds represented by formulas (1) to (3);
xLiNi aCobMcO2·(1-x)Li2MnO3 formula (1);
xLiMn aM2-aO4·(1-x)Li2MnO3 formula (2);
LiNi xCoyMnzM1-x-y-zO2 formula (3);
in the formula (1), the components are as follows, 0 < x <1, 0 < a <1, 0b is more than or equal to 1, 0c is more than or equal to 1;
In the formula (2), the amino acid sequence of the compound, 0 < x < 1, 0a is more than or equal to 1;
In the formula (3), the amino acid sequence of the compound, y is more than or equal to 0 and less than or equal to 1,0 x is more than or equal to 1,0 z is more than or equal to 1, and x+y+z is more than or equal to 1;
m is any one of Fe, co, ni, mn, mg, cu, zn, al, sn, cd, B, ga, cr, sr, V, ti, mo, W, sb, zr, nb, bi respectively and independently.
More preferably, the lithium-containing material is selected from one or a combination of two or more of LiNiO2、0.7LiNi0.5Mn0.5O2·0.3Li2MnO3、0.5LiCoO2·0.5Li2MnO3、0.5LiMn1.5Ni0.5O4·0.5Li2MnO3.
Preferably, the positive electrode includes an active material layer including the positive electrode active material, and an insulating coating layer coated on a surface of the active material layer. The insulating coating coated on the surface of the positive electrode can improve the thermal stability of the positive electrode plate, thereby improving the safety performance of the system.
Further preferably, the insulating coating is mainly composed of the following components in percentage by mass: 60-99% of inorganic ceramic material and 1-40% of binder. The sum of the mass fractions of the inorganic ceramic material and the binder is 100 percent.
More preferably, the inorganic ceramic material is any one or more of alumina, titania, zinc oxide, zirconium dioxide, tin dioxide, magnesium oxide, silica, boehmite; the binder is one or more of polyvinylidene fluoride, acrylic esters, acrylic acid, polyvinyl alcohol, carboxymethyl fibers and polyurethane. The thickness of the insulating coating is 1-20 mu m.
Preferably, the electrolyte consists of an organic solvent, an electrolyte salt and a functional additive, wherein the functional additive is selected from one or more of vinylene carbonate, fluoroethylene carbonate, 1, 3-propane sultone, ethylene sulfate, propylene sultone, lithium bisoxalato borate, lithium difluorooxalato borate, lithium difluorobisoxalato phosphate, lithium tetrafluorooxalato phosphate, lithium tetrafluoroborate, methylene methane disulfonate, tris (trimethylsilane) borate and tris (trimethylsilane) phosphate.
Further preferably, the functional additive consists of Vinylene Carbonate (VC), 1, 3-Propane Sultone (PS) and lithium difluorooxalato borate (LiODFB) according to a mass ratio of 1.5:1:1.5, or consists of Vinylene Carbonate (VC), propenesulfonic acid lactone (PST) and lithium difluorooxalato borate (LiODFB) according to a mass ratio of 1.5:0.6:1.5. The liquid electrolyte is adopted, so that the ion migration rate is higher and the anode and cathode compatibility is better.
Detailed Description
The invention hopes to prepare the non-negative electrode lithium secondary battery with energy density and cycle performance, which not only avoids the safety risk caused by using a metal lithium sheet in the battery manufacturing process, but also improves the problem of poor cycle of the non-negative electrode battery using the traditional positive electrode material.
The preparation method of the non-negative electrode lithium secondary battery comprises the following steps:
1) Preparation of positive electrode: adding the lithium-containing material with the initial effect lower than 85%, the conductive agent and the binder into a solvent, and uniformly mixing to obtain anode slurry; uniformly coating the anode slurry on an anode current collector, drying, uniformly coating the insulating coating slurry on the surface of the anode, wherein the thickness of the insulating coating slurry is 1-20 mu m, and rolling to obtain an anode;
Preparation of insulating coating slurry: dissolving a certain amount of binder in NMP, stirring until the binder is transparent for standby, adding inorganic ceramic material and a proper amount of NMP according to a certain proportion, adding a small amount of dispersing agent, stirring for 30min, adding the binder glue solution, and stirring for 30min again to obtain the composite ceramic material;
Preparation of the negative electrode: the negative electrode is a negative electrode current collector without negative electrode material, more preferably copper foil, copper-plated composite film and the like;
2) And (3) assembling a battery cell: forming a battery core assembly by the positive electrode, the diaphragm and the negative electrode lamination, and filling the battery core assembly into a shell;
3) Injection of electrolyte: and injecting liquid electrolyte into the battery shell to obtain the non-negative electrode lithium secondary battery.
In the positive electrode slurry, the solvent is N-methyl pyrrolidone, the conductive agent is conductive carbon black or conductive slurry, and the binder is polyvinylidene fluoride (PVDF). The active material layer consists of a lithium-containing material, a conductive agent and a binder according to the mass ratio of 92-96:1-3:2-5. Preferably 95:2:3.
The diaphragm is any one of a polypropylene diaphragm, a polyethylene diaphragm, an inorganic ceramic coating diaphragm, a glass fiber non-woven fabric diaphragm, a polypropylene and polyethylene composite ceramic diaphragm and the like.
The liquid electrolyte consists of an organic solvent, electrolyte salt and a functional additive.
The organic solvent is any one of ethylene carbonate, diethyl carbonate, dimethyl carbonate, propylene carbonate, methyl ethyl carbonate, methyl formate, methyl acetate, ethyl butyrate and methyl butyrate; preferably Ethylene Carbonate (EC), ethylmethyl carbonate (EMC) and diethyl carbonate (DEC) according to the volume ratio of 2-4:4-6:1-3. More preferably 3:5:2.
The electrolyte salt is any one or a combination of lithium hexafluorophosphate (LiPF 6), lithium bis (fluorosulfonyl) imide and lithium bis (trifluoromethylsulfonyl) imide.
Embodiments of the present invention will be further described with reference to the following specific examples.
1. Specific examples of non-negative lithium Secondary Battery
Example 1
The non-negative electrode lithium secondary battery of the present embodiment includes a positive electrode (1), a negative electrode (2), a separator (3), and an electrolyte (4).
(1) Positive electrode
The positive electrode includes an active material layer coated on the positive electrode current collector and an insulating coating layer coated on the active material layer.
The active material layer is composed of lithium-containing material with initial effect lower than 85%, conductive agent and binder. The lithium-containing material is LiNiO 2, and the conductive agent is carbon black. The binder is polyvinylidene fluoride (PVDF). The mass ratio of the lithium-containing material LiNiO 2, the conductive agent carbon black and the binder polyvinylidene fluoride (PVDF) is 95:2:3.
The insulating coating mainly comprises inorganic ceramic material and binder (the other components are a little dispersant), wherein the inorganic ceramic material SiO 2 accounts for 93% and the binder polyvinylidene fluoride (PVDF) accounts for 7%.
(2) Negative electrode
The negative electrode is a current collector without active material, specifically copper foil, before the battery is charged and discharged.
(3) Diaphragm
The diaphragm is a ceramic diaphragm sold in the market.
(4) Electrolyte solution
The electrolyte consists of an organic solvent, electrolyte salt and a functional additive.
The organic solvent consists of EC, EMC, DEC in a volume ratio of 3:5:2.
The electrolyte salt was LiPF 6, and the concentration in the electrolyte was 1.2mol/L.
The functional additive consists of VC, PS, liODFB percent by mass and the mass ratio of the functional additive in the electrolyte is 1.5 percent, 1 percent and 1.5 percent respectively.
The manufacturing method of the non-negative electrode lithium secondary battery of the present embodiment is as follows:
Adding a positive electrode lithium-containing material LiNiO 2, a conductive agent carbon black and a binder polyvinylidene fluoride (PVDF) into a solvent N-methylpyrrolidone, and uniformly mixing the materials to obtain a positive electrode slurry, wherein the mass ratio of the positive electrode lithium-containing material LiNiO 2 to the conductive agent carbon black to the binder polyvinylidene fluoride (PVDF) is 95:2:3; uniformly coating the anode slurry on an anode current collector Al foil, drying, uniformly coating the insulating coating slurry on the surface of the anode, and rolling to obtain an anode; wherein the thickness of the insulating coating layer coated on the positive electrode slurry was 10 μm.
The insulating coating paste was prepared as follows: the slurry consists of inorganic ceramic material and binder, wherein the inorganic ceramic material comprises 93% of SiO 2 and 7% of binder polyvinylidene fluoride (PVDF), the PVDF is dissolved in NMP, and the mixture is stirred to be transparent for standby, the SiO 2 is added with a proper amount of NMP, a little dispersant polyvinylpyrrolidone (PVP for short) is added, the addition amount is 0.5%, and the mixture is stirred for 30min, and then the binder glue solution is added and stirred for 30min to obtain the composite material.
The diaphragm is a ceramic diaphragm; the liquid electrolyte is a mixed solution composed of solvent EC/EMC/dec=3/5/2, lipf 6 1.2.2M and additive VC, PS, liODFB.
Laminating the anode, the ceramic diaphragm and the cathode copper foil to form a cell assembly, and loading the cell assembly into a shell; and injecting liquid electrolyte to obtain the non-negative electrode lithium secondary battery.
Example 2
The non-negative electrode lithium secondary battery of this example was different from that described in example 1 in that the positive electrode active material was 0.7LiNi 0.5Mn0.5O2·0.3Li2MnO3, and the other points not described were the same as in example 1.
Example 3
The non-negative electrode lithium secondary battery of this example was different from that described in example 1 in that the positive electrode active material was 0.5LiCoO 2·0.5Li2MnO3, and the other points not described were the same as in example 1.
Example 4
The non-negative electrode lithium secondary battery of this example was different from that described in example 1 in that the positive electrode active material was 0.5LiMn 1.5Ni0.5O4·0.5Li2MnO3, and the other points not described were the same as in example 1.
Example 5
The non-negative electrode lithium secondary battery of this example is different from that described in example 1 in that the positive electrode active material is a mixed positive electrode material composed of 0.7LiNi 0.5Mn0.5O2·0.3Li2MnO3 and LiNiO 2, and the mass ratio of the two is 8:2, the other points not described are the same as those in example 1.
Example 6
The non-negative lithium secondary battery of this example is different from that described in example 2 in that the electrolyte solution adopts the following electrolyte solution scheme.
The electrolyte consists of an organic solvent, electrolyte salt and a functional additive.
The organic solvent consists of EC, EMC, DEC in a volume ratio of 3:5:2.
The electrolyte salt was LiPF6, and the concentration in the electrolyte was 1.2mol/L.
The functional additive consists of VC, PST, liODFB percent by mass and the mass ratio of the functional additive in the electrolyte is 1.5 percent, 0.6 percent and 1.5 percent respectively.
The other points not described are the same as in example 2.
Table 1 list of embodiments
2. Comparative example
Comparative example 1
The method for manufacturing the negative electrode-free lithium secondary battery of the comparative example is as follows:
Adding a positive electrode material LiCoO 2, a conductive agent carbon black and a binder polyvinylidene fluoride (PVDF) into a solvent N-methylpyrrolidone, wherein the mass ratio of the positive electrode material LiCoO 2 to the conductive agent carbon black to the binder polyvinylidene fluoride (PVDF) is 95:2:3, and uniformly mixing to obtain a positive electrode slurry; uniformly coating the anode slurry on an anode current collector Al foil, drying, uniformly coating the insulating coating slurry on the surface of the anode, and rolling to obtain an anode (the preparation of the insulating coating slurry is the same as that of example 1); wherein the thickness of the insulating coating layer coated on the positive electrode slurry was 10 μm.
Laminating the anode, the ceramic diaphragm and the cathode copper foil to form a cell assembly, and loading the cell assembly into a shell; and (3) injecting a liquid electrolyte (the same as in example 1) to obtain the non-negative electrode lithium secondary battery.
3. Experimental example
The non-negative lithium secondary batteries prepared according to each example and comparative example were cycled between 2.5V-4.8V at 0.1C charge/0.1C discharge for 1 time, and then subjected to a normal temperature cycle test of 0.1C charge/0.2C discharge between 2.8V-4.4V, and the first coulombic efficiency (charge/discharge efficiency of 0.1C charge/0.1C discharge) and the 20-cycle capacity retention (20 th discharge capacity/0.2C first discharge capacity) of each group were recorded, and the results of each group are shown in table 2 below.
Table 2 battery test results for examples and comparative examples
As can be seen from the above table, the first efficiency of each of the embodiments is lower than that of the comparative example, but the capacity retention rate after 20 cycles is much higher than that of the comparative example, indicating that the non-negative lithium secondary battery adopting the positive electrode scheme of the present invention greatly improves the cycle performance of the non-negative lithium secondary battery.
Claims (9)
1. The non-negative electrode lithium secondary battery is characterized by comprising a positive electrode, a negative electrode, a diaphragm and electrolyte, wherein a positive electrode active material of the positive electrode is a lithium-containing material with the first efficiency lower than 85%;
The lithium-containing material is selected from one or more than two of compounds shown in the formulas (1) to (2);
xLiNi aCobMcO2·(1-x)Li2MnO3 formula (1);
xLiMn aM2-aO4·(1-x)Li2MnO3 formula (2);
in the formula (1), the components are as follows, 0 < x <1, 0 < a <1, 0b is more than or equal to 1, 0c is more than or equal to 1;
In the formula (2), the amino acid sequence of the compound, 0 < x < 1, 0a is more than or equal to 1;
m is any one of Fe, co, ni, mn, mg, cu, zn, al, sn, cd, B, ga, cr, sr, V, ti, mo, W, sb, zr, nb, bi respectively and independently.
2. The negative electrode-less lithium secondary battery according to claim 1, wherein the first efficiency of the positive electrode active material is not less than 60% and not more than 82%.
3. The negative electrode-less lithium secondary battery according to claim 1, wherein the lithium-containing material is selected from one or a combination of two or more kinds of 0.7LiNi0.5Mn0.5O2·0.3Li2MnO3、0.5LiCoO2·0.5Li2MnO3、0.5LiMn1.5Ni0.5O4·0.5Li2MnO3.
4. The negative-electrode-free lithium secondary battery according to any one of claims 1 to 3, wherein the positive electrode comprises an active material layer containing the positive electrode active material, and an insulating coating layer coated on a surface of the active material layer.
5. The negative electrode-less lithium secondary battery according to claim 4, wherein the insulating coating layer is mainly composed of the following components by mass: 60-99% of inorganic ceramic material and 1-40% of binder.
6. The non-negative electrode lithium secondary battery according to claim 5, wherein the inorganic ceramic material is any one or more of alumina, titania, zinc oxide, zirconia, tin dioxide, magnesia, silica, boehmite; the binder is one or more of polyvinylidene fluoride, acrylic esters, acrylic acid, polyvinyl alcohol, carboxymethyl fibers and polyurethane.
7. The negative electrode-less lithium secondary battery according to claim 4, wherein the thickness of the insulating coating layer is 1 to 20 μm.
8. The negative electrode-free lithium secondary battery according to any one of claims 1 to 3, wherein the electrolyte is composed of an organic solvent, an electrolyte salt, and a functional additive selected from one or more of vinylene carbonate, fluoroethylene carbonate, 1, 3-propane sultone, vinyl sulfate, propenesulfonic acid lactone, lithium bisoxalato borate, lithium difluorooxalato borate, lithium difluorobisoxalato phosphate, lithium tetrafluorooxalato phosphate, lithium tetrafluoroborate, methylene methane disulfonate, tris (trimethylsilane) borate, and tris (trimethylsilane) phosphate.
9. The negative electrode-less lithium secondary battery according to claim 8, wherein the functional additive is composed of vinylene carbonate, 1, 3-propane sultone and lithium difluorooxalato borate in a mass ratio of 1.5:1:1.5 or is composed of vinylene carbonate, propenesulfonic acid lactone and lithium difluorooxalato borate in a mass ratio of 1.5:0.6:1.5.
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