CN111584860A - High specific energy cylindrical lithium ion battery and preparation method thereof - Google Patents
High specific energy cylindrical lithium ion battery and preparation method thereof Download PDFInfo
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- CN111584860A CN111584860A CN202010264837.2A CN202010264837A CN111584860A CN 111584860 A CN111584860 A CN 111584860A CN 202010264837 A CN202010264837 A CN 202010264837A CN 111584860 A CN111584860 A CN 111584860A
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- lithium ion
- ion battery
- specific energy
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 45
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 45
- 238000002360 preparation method Methods 0.000 title abstract description 7
- 239000000463 material Substances 0.000 claims abstract description 31
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 29
- 239000006258 conductive agent Substances 0.000 claims abstract description 21
- 239000003792 electrolyte Substances 0.000 claims abstract description 21
- 239000013543 active substance Substances 0.000 claims abstract description 19
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 17
- 239000007773 negative electrode material Substances 0.000 claims abstract description 14
- 239000002134 carbon nanofiber Substances 0.000 claims abstract description 12
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 12
- 239000002033 PVDF binder Substances 0.000 claims abstract description 10
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims abstract description 10
- 239000007774 positive electrode material Substances 0.000 claims abstract description 10
- 239000001768 carboxy methyl cellulose Substances 0.000 claims abstract description 9
- 229920000049 Carbon (fiber) Polymers 0.000 claims abstract description 7
- 239000004917 carbon fiber Substances 0.000 claims abstract description 7
- 229920003048 styrene butadiene rubber Polymers 0.000 claims abstract description 7
- 229920002134 Carboxymethyl cellulose Polymers 0.000 claims abstract description 6
- 235000010948 carboxy methyl cellulose Nutrition 0.000 claims abstract description 6
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 claims abstract description 4
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 claims abstract description 4
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 claims abstract description 4
- 239000011248 coating agent Substances 0.000 claims description 32
- 238000000576 coating method Methods 0.000 claims description 32
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical class [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 21
- 239000002002 slurry Substances 0.000 claims description 18
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 17
- 229910052782 aluminium Inorganic materials 0.000 claims description 17
- 238000000034 method Methods 0.000 claims description 13
- 239000002041 carbon nanotube Substances 0.000 claims description 12
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 12
- 239000011888 foil Substances 0.000 claims description 12
- 239000002904 solvent Substances 0.000 claims description 12
- 239000011267 electrode slurry Substances 0.000 claims description 11
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 10
- 239000011230 binding agent Substances 0.000 claims description 10
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 10
- 238000005096 rolling process Methods 0.000 claims description 10
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 8
- 239000011889 copper foil Substances 0.000 claims description 8
- 239000002245 particle Substances 0.000 claims description 8
- 239000000654 additive Substances 0.000 claims description 7
- 230000000996 additive effect Effects 0.000 claims description 7
- 238000002156 mixing Methods 0.000 claims description 7
- 238000001035 drying Methods 0.000 claims description 6
- 239000007772 electrode material Substances 0.000 claims description 6
- 229920000139 polyethylene terephthalate Polymers 0.000 claims description 6
- 239000005020 polyethylene terephthalate Substances 0.000 claims description 6
- 238000001947 vapour-phase growth Methods 0.000 claims description 6
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 5
- 229910013872 LiPF Inorganic materials 0.000 claims description 5
- 101150058243 Lipf gene Proteins 0.000 claims description 5
- 239000008112 carboxymethyl-cellulose Substances 0.000 claims description 5
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 5
- 239000003960 organic solvent Substances 0.000 claims description 5
- 239000000377 silicon dioxide Substances 0.000 claims description 5
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 5
- 239000012498 ultrapure water Substances 0.000 claims description 5
- 238000003466 welding Methods 0.000 claims description 5
- 238000004804 winding Methods 0.000 claims description 5
- 239000010439 graphite Substances 0.000 claims description 4
- 229910002804 graphite Inorganic materials 0.000 claims description 4
- 125000001140 1,4-phenylene group Chemical group [H]C1=C([H])C([*:2])=C([H])C([H])=C1[*:1] 0.000 claims description 3
- CQPBLBQMIFRGLU-UHFFFAOYSA-N 4-(6-azabicyclo[3.1.1]hepta-1(7),2,4-triene-6-carbonyl)benzamide Chemical compound C1=CC(C(=O)N)=CC=C1C(=O)N1C2=CC=CC1=C2 CQPBLBQMIFRGLU-UHFFFAOYSA-N 0.000 claims description 3
- 229910000831 Steel Inorganic materials 0.000 claims description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 3
- 229910003481 amorphous carbon Inorganic materials 0.000 claims description 3
- 239000010405 anode material Substances 0.000 claims description 3
- 229910052681 coesite Inorganic materials 0.000 claims description 3
- 229910052593 corundum Inorganic materials 0.000 claims description 3
- 229910052906 cristobalite Inorganic materials 0.000 claims description 3
- 238000004806 packaging method and process Methods 0.000 claims description 3
- 239000003973 paint Substances 0.000 claims description 3
- -1 polyethylene terephthalate Polymers 0.000 claims description 3
- 239000010959 steel Substances 0.000 claims description 3
- 229910052682 stishovite Inorganic materials 0.000 claims description 3
- 239000000758 substrate Substances 0.000 claims description 3
- 229910052905 tridymite Inorganic materials 0.000 claims description 3
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 3
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052710 silicon Inorganic materials 0.000 claims description 2
- 239000010703 silicon Substances 0.000 claims description 2
- 239000002174 Styrene-butadiene Substances 0.000 abstract description 3
- 239000012808 vapor phase Substances 0.000 abstract 1
- 210000004027 cell Anatomy 0.000 description 14
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 8
- 230000008569 process Effects 0.000 description 7
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 5
- 229910000480 nickel oxide Inorganic materials 0.000 description 5
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 5
- 239000012071 phase Substances 0.000 description 5
- 238000007086 side reaction Methods 0.000 description 5
- 235000002639 sodium chloride Nutrition 0.000 description 5
- 239000011780 sodium chloride Substances 0.000 description 5
- 229910018553 Ni—O Inorganic materials 0.000 description 4
- 238000005056 compaction Methods 0.000 description 4
- 239000013078 crystal Substances 0.000 description 4
- 238000002347 injection Methods 0.000 description 4
- 239000007924 injection Substances 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 230000009466 transformation Effects 0.000 description 4
- 230000014759 maintenance of location Effects 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 229910052493 LiFePO4 Inorganic materials 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- 239000006257 cathode slurry Substances 0.000 description 2
- 238000005520 cutting process Methods 0.000 description 2
- 210000001787 dendrite Anatomy 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 238000004146 energy storage Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 229910052744 lithium Inorganic materials 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 229920000131 polyvinylidene Polymers 0.000 description 2
- 230000001105 regulatory effect Effects 0.000 description 2
- 238000007789 sealing Methods 0.000 description 2
- 229910012820 LiCoO Inorganic materials 0.000 description 1
- 229910032387 LiCoO2 Inorganic materials 0.000 description 1
- 229910013716 LiNi Inorganic materials 0.000 description 1
- PFYQFCKUASLJLL-UHFFFAOYSA-N [Co].[Ni].[Li] Chemical compound [Co].[Ni].[Li] PFYQFCKUASLJLL-UHFFFAOYSA-N 0.000 description 1
- 239000006256 anode slurry Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000007770 graphite material Substances 0.000 description 1
- 238000009863 impact test Methods 0.000 description 1
- 238000007689 inspection Methods 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 239000002210 silicon-based material 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
- 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
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
-
- 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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0569—Liquid materials characterised by the solvents
-
- 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
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
-
- 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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
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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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
- H01M2300/004—Three solvents
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- 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
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention belongs to the field of lithium ion batteries, and particularly relates to a high-specific-energy cylindrical lithium ion battery and a preparation method thereof, wherein the high-specific-energy cylindrical lithium ion battery comprises a positive electrode material, a negative electrode material, electrolyte and a diaphragm, the positive electrode material comprises 94-98% by mass of an active substance, 1-3% by mass of a conductive agent and 1-3% by mass of polyvinylidene fluoride, the active substance is a Mg-doped modified high-nickel NCA material, the conductive agent comprises conductive carbon black SP and vapor-phase grown carbon fiber VGCF, and the negative electrode material comprises 88-94% by mass of an active substance, 2-6% by mass of a conductive agent, 1-3% by mass of sodium carboxymethylcellulose CMC and 1-3% by mass of styrene butadiene rubber SBR. The invention provides a high-specific-energy cylindrical lithium ion battery with high specific energy, high safety, long cycle life and excellent low-temperature discharge performance and a preparation method thereof.
Description
Technical Field
The invention belongs to the field of lithium ion batteries, and particularly relates to a high specific energy cylindrical lithium ion battery and a preparation method thereof.
Background
The prior art and the defects are as follows:
in recent years, with the continuous update and upgrade of military and civil energy storage systems, people put higher requirements on the energy density of lithium ion batteries. LiCoO currently in the market2C and LiFePO4the/C electrode material system cannot meet the development requirement of the high specific energy lithium ion battery.
The layered nickel cobalt lithium aluminate (NCA) material with high nickel content has higher theoretical capacity, however, in the actual circulation process, the surface of the high nickel NCA material is easy to generate side reaction of electrolyte to generate inert rock salt phase nickel oxide so as to cause rapid capacity attenuation; the existing high-nickel NCA material needs to be modified by doping, surface coating, etc. to improve the cycle performance. In addition, the safety performance of high-nickel NCA materials is compatible with LiCoO2And LiFePO4The difference is large, so that the safety performance of the nickel NCA system battery needs to be improved through various modifications of electrode materials, electrolyte, a diaphragm and the like.
Compared with the traditional graphite material, the high-capacity silicon (Si)/silicon monoxide (SiO) with a certain proportion is preparedx) The blending of the material and graphite can significantly improve the capacity of the negative electrode. However, the silicon-based material generally has the problem of volume expansion, and needs to be modified in the aspects of electrode materials, electrolyte and the like
The difficulty and significance for solving the technical problems are as follows:
therefore, based on these problems, it is important to provide a high specific energy cylindrical lithium ion battery with high specific energy, high safety, long cycle life and excellent low-temperature discharge performance, and a preparation method thereof.
Disclosure of Invention
The invention aims to solve the technical problems in the prior art and provide a high-specific-energy cylindrical lithium ion battery with high specific energy, high safety, long cycle life and excellent low-temperature discharge performance and a preparation method thereof.
The technical scheme adopted by the invention for solving the technical problems in the prior art is as follows:
a high specific energy cylindrical lithium ion battery comprises a positive electrode material, a negative electrode material, an electrolyte and a diaphragm,
the positive electrode material comprises 94-98% of active substance, 1-3% of conductive agent and 1-3% of polyvinylidene fluoride (PVDF, binder) by mass, the active substance is Mg-doped modified high-nickel NCA material, the conductive agent comprises conductive carbon black SP and vapor phase growth carbon fiber VGCF (polyvinylidene fluoride-polyvinylidene fluoride), and the mass ratio of the conductive carbon black SP to the vapor phase growth carbon fiber VGCF is MSP:MVGCF＝0.5-2；
The doping of trace Mg on the surface can stabilize the Ni-O bond of NCA and inhibit the generation of rock salt phase nickel oxide transformation side reaction, thereby effectively maintaining the layered crystal structure of the NCA material in the circulating process and improving the circulating stability of the material.
The negative electrode material comprises, by mass, 88-94% of an active substance, 2-6% of a conductive agent, 1-3% of sodium carboxymethylcellulose (CMC), 1-3% of Styrene Butadiene Rubber (SBR) (a binder), 92-96% of a modified graphite and 4-8% of silicon monoxide, the graphite is modified by coating a nano-thick amorphous carbon layer on the surface, the conductive agent comprises Carbon Nanotube (CNT) and conductive carbon black (SP), and the mass ratio of the Carbon Nanotube (CNT) to the conductive carbon black (SP) is MSP:MCNT＝0.5-2；
The electrolyte comprises electrolyte LiPF with the concentration of 0.8-1.3mol/L6The paint comprises ethylene carbonate EC accounting for 20-40% of the solvent volume fraction, ethyl methyl carbonate EMC accounting for 20-40%, dimethyl carbonate DMC mixed organic solvent accounting for 20-40% of the solvent volume fraction, and a film forming additive;
the battery diaphragm is a coating diaphragm taking polyethylene terephthalate (PET) as a substrate, and the coating comprises SiO2、Al2O3Or poly (p-phenylene/m-phenylene terephthalamide).
The coating diaphragm technology can effectively improve the safety performance of the battery.
The invention aims to provide a design scheme of a high-specific-energy lithium ion cylindrical battery, which has high specific energy, high safety, long cycle life and excellent low-temperature discharge performance.
The invention can also adopt the following technical scheme:
in the cylindrical lithium ion battery with high specific energy, furthermore, the current collector used by the anode is an aluminum foil with the thickness of 10-20 μm, and the cathode is a copper foil with the thickness of 6-10 μm; the density of the double-sided coating surface of the positive electrode is 40-46mg/cm2The density of the double-sided coating surface of the negative electrode is 20-24mg/cm2(ii) a The compacted density of the anode material is 3.4-3.8g/cm3The compacted density of the negative electrode material is 0.8-1.5g/cm3。
The thickness of the aluminum foil, the material compaction density, the coating surface density, and the like are defined in order to optimize the energy density of the battery, and the thinner the aluminum foil, the higher the compaction density and the higher the coating surface density, the higher the energy density, but the lower the cycle performance safety performance is caused, and an optimal value needs to be found.
In the above cylindrical lithium ion battery with high specific energy, further, the positive electrode active material is a high nickel NCA material doped with Mg and coated with surface oxide, LiNi0.91-xCo0.07Al0.02MgxO2Wherein the Mg mole fraction x is 0.005-0.02, the LiNi0.91-xCo0.07Al0.02MgxO2Has a particle diameter of 12-15 μm and a specific surface area of 0.4-0.6m2/g。
The doping of trace Mg on the surface can stabilize the Ni-O bond of NCA and inhibit the generation of rock salt phase nickel oxide transformation side reaction, thereby effectively maintaining the layered crystal structure of the NCA material in the circulating process and improving the circulating stability of the material.
The particle size and the specific surface area are intrinsic parameters of the material, cannot be regulated and controlled, and are only limited in range.
In the cylindrical lithium ion battery with high specific energy, furthermore, the value of the anode capacity ratio N/P of the electrode material is 1.0-2.0,
the significance of the capacity proportioning coefficient of the anode and the cathode lies in the reasonable utilization of active lithium ions. If the positive electrode is excessive, lithium dendrite is formed on the surface of the negative electrode in the charging process; if the negative electrode is too excessive, the first round charging and discharging efficiency is too low.
In the cylindrical lithium ion battery with high specific energy, furthermore, the particle diameter d50 of the negative active material is 10-20 μm, and the specific surface area is 1-2m2/g。
In the cylindrical lithium ion battery with high specific energy, the viscosity of the anode electrode slurry and the cathode electrode slurry is 1500-.
In the above cylindrical lithium ion battery with high specific energy, further, the battery case is a steel case or an aluminum case.
A method of making a high specific energy lithium ion battery, comprising the steps of:
the method comprises the following steps: mixing a positive active substance, a conductive agent and a binder into slurry by taking NMP as a solvent, uniformly coating the slurry on the surface of an aluminum foil, and drying, rolling and slitting the slurry to prepare a pole piece;
step two: mixing a negative electrode active substance, a conductive agent and a binder into slurry by taking ultrapure water as a solvent, uniformly coating the slurry on the surface of copper foil, and drying, rolling and slitting the slurry to prepare a pole piece;
step three: preparing the prepared positive plate, the prepared negative plate and the diaphragm into a battery cell in a winding mode, ensuring that a negative electrode in the material attachment area wraps a positive electrode, fixing tabs of the positive electrode and the negative electrode by welding, and finally packaging into a dry battery cell; injecting a certain amount of electrolyte into the battery cell; and (3) forming the battery cell to obtain the cylindrical lithium ion battery with high specific energy.
In conclusion, the invention has the following advantages and positive effects:
1. the high specific energy cylindrical lithium ion battery prepared by the invention has ultrahigh weight specific energy, good cycle performance and excellent safety performance, and can be used in the field of energy storage and conversion with higher requirements on safety performance and specific energy.
2. The cylindrical lithium ion battery prepared by the invention has high specific energy, and the energy density of the single battery is more than 280Wh/kg, so that the requirement of various energy systems on the energy density can be met.
3. The lithium ion battery prepared by the invention has excellent cycle performance, the discharge depth is more than or equal to 90%, the cycle can be carried out for more than 400 circles, and the capacity retention rate is more than 80%.
4. The lithium ion battery prepared by the invention has excellent low-temperature discharge performance, and is discharged in the environment after being placed in a low-temperature box at the temperature of minus 25 ℃ for 8 hours after being fully charged, and the discharge capacity is not lower than 80% of the rated capacity.
5. The lithium ion battery prepared by the invention has excellent safety performance. The battery is subjected to vibration and impact tests, and the discharge current and the discharge voltage of the battery have no sudden change and no mechanical damage in the tests. The battery is subjected to thermal vacuum inspection, and the battery is not deformed, cracked and leaked. The battery is tested for short circuit, overcharge and overdischarge, and the battery does not catch fire or explode.
Detailed Description
A high specific energy cylindrical lithium ion battery comprises a positive electrode material, a negative electrode material, an electrolyte and a diaphragm,
the positive electrode material comprises 94-98% of active substance, 1-3% of conductive agent and 1-3% of polyvinylidene fluoride (PVDF, binder) by mass, the active substance is Mg-doped modified high-nickel NCA material, the conductive agent comprises conductive carbon black SP and vapor phase growth carbon fiber VGCF (polyvinylidene fluoride-polyvinylidene fluoride), and the mass ratio of the conductive carbon black SP to the vapor phase growth carbon fiber VGCF is MSP:MVGCF＝0.5-2；
The doping of trace Mg on the surface can stabilize the Ni-O bond of NCA and inhibit the generation of rock salt phase nickel oxide transformation side reaction, thereby effectively maintaining the layered crystal structure of the NCA material in the circulating process and improving the circulating stability of the material.
The negative electrode material comprises, by mass, 88-94% of an active substance, 2-6% of a conductive agent, 1-3% of sodium carboxymethylcellulose (CMC), 1-3% of Styrene Butadiene Rubber (SBR) (a binder), 92-96% of a modified graphite and 4-8% of silicon monoxide, the graphite is modified by coating a nano-thick amorphous carbon layer on the surface, the conductive agent comprises Carbon Nanotube (CNT) and conductive carbon black (SP), and the mass ratio of the Carbon Nanotube (CNT) to the conductive carbon black (SP) is MSP:MCNT＝0.5-2；
The electrolyte comprises electrolyte LiPF with the concentration of 0.8-1.3mol/L6The paint comprises ethylene carbonate EC accounting for 20-40% of the solvent volume fraction, ethyl methyl carbonate EMC accounting for 20-40%, dimethyl carbonate DMC mixed organic solvent accounting for 20-40% of the solvent volume fraction, and a film forming additive;
the battery diaphragm is a coating diaphragm taking polyethylene terephthalate (PET) as a substrate, and the coating comprises SiO2、Al2O3Or poly (p-phenylene/m-phenylene terephthalamide).
The coating diaphragm technology can effectively improve the safety performance of the battery.
The invention aims to provide a design scheme of a high-specific-energy lithium ion cylindrical battery, which has high specific energy, high safety, long cycle life and excellent low-temperature discharge performance.
Still further, it is also contemplated in the present invention that the current collector for the positive electrode is an aluminum foil with a thickness of 10-20 μm, and the negative electrode is a copper foil with a thickness of 6-10 μm; the density of the double-sided coating surface of the anode is 40-46mg/cm2The density of the double-sided coating surface of the negative electrode is 20-24mg/cm2(ii) a The compacted density of the anode material is 3.4-3.8g/cm3The compacted density of the negative electrode material is 0.8-1.5g/cm3。
The thickness of the aluminum foil, the material compaction density, the coating surface density, and the like are defined in order to optimize the energy density of the battery, and the thinner the aluminum foil, the higher the compaction density and the higher the coating surface density, the higher the energy density, but the lower the cycle performance safety performance is caused, and an optimal value needs to be found.
Still further, it is also contemplated in the present invention that the positive electrode active material is a high nickel NCA material doped with Mg and coated with a surface oxide, LiNi0.91-xCo0.07Al0.02MgxO2Wherein the Mg mole fraction x is 0.005-0.02, the LiNi0.91-xCo0.07Al0.02MgxO2Has a particle diameter of 12-15 μm and a specific surface area of 0.4-0.6m2/g。
The doping of trace Mg on the surface can stabilize the Ni-O bond of NCA and inhibit the generation of rock salt phase nickel oxide transformation side reaction, thereby effectively maintaining the layered crystal structure of the NCA material in the circulating process and improving the circulating stability of the material.
The particle size and the specific surface area are intrinsic parameters of the material, cannot be regulated and controlled, and are only limited in range.
Still further, it is also contemplated in the present invention that the electrode material has a negative electrode-positive electrode capacity ratio N/P value of 1.0 to 2.0,
the significance of the capacity proportioning coefficient of the anode and the cathode lies in the reasonable utilization of active lithium ions. If the positive electrode is excessive, lithium dendrite is formed on the surface of the negative electrode in the charging process; if the negative electrode is too excessive, the first round charging and discharging efficiency is too low.
It is noted that the particle diameter d50 of the negative electrode active material is 10 to 20 μm, and the specific surface area is 1 to 2m2/g。
The viscosity of the positive electrode slurry and the negative electrode slurry is 1500-6000 mPa.S, and the battery electrolyte film-forming additive is one or two of FEC and VC.
It should be noted that the battery case is a steel case or an aluminum case.
A method of making a high specific energy lithium ion battery, comprising the steps of:
the method comprises the following steps: mixing a positive active substance, a conductive agent and a binder into slurry by taking NMP as a solvent, uniformly coating the slurry on the surface of an aluminum foil, and drying, rolling and slitting the slurry to prepare a pole piece;
step two: mixing a negative electrode active substance, a conductive agent and a binder into slurry by taking ultrapure water as a solvent, uniformly coating the slurry on the surface of copper foil, and drying, rolling and slitting the slurry to prepare a pole piece;
step three: preparing the prepared positive plate, the prepared negative plate and the diaphragm into a battery cell in a winding mode, ensuring that a negative electrode in the material attachment area wraps a positive electrode, fixing tabs of the positive electrode and the negative electrode by welding, and finally packaging into a dry battery cell; injecting a certain amount of electrolyte into the battery cell; and (3) forming the battery cell to obtain the cylindrical lithium ion battery with high specific energy.
In order to further understand the contents, features and effects of the present invention, the following examples are illustrated, and the following detailed descriptions are given:
example 1:
modifying LiNi by 95 wt% to obtain LiNi0.805Co0.07Al0.02Mg0.015O2And 1 wt% of conductive carbon black, 1 wt% of vapor grown carbon fiber and 3 wt% of PVDF are respectively dissolved in NMP to prepare anode slurry.
The negative electrode slurry was prepared by dissolving a mixed material of 87.4 wt% of modified graphite and 4.6 wt% of silica, 2 wt% of conductive carbon black, 2 wt% of carbon nanotubes, 2 wt% of CMC, and 2 wt% of SBR in ultrapure water, respectively.
The positive electrode slurry is uniformly coated on the surface of an aluminum foil with the thickness of 12 mu m, and the density of double surfaces is 42mg/cm2The compacted density after one-time rolling is 3.5g/cm3(ii) a The cathode slurry is uniformly coated on the surface of a copper foil with the thickness of 8 mu m, and the density of two surfaces is 22mg/cm2The compacted density after one-time rolling is 1.3g/cm3。
Cutting the positive and negative electrode plates, winding into electric core, and coating Al with thickness of 16 μm between the positive and negative electrodes2O3The coating diaphragm is separated, the anode and cathode tabs of the anode and the cathode are wrapped by the cathode in the auxiliary material area and are fixed by welding, and finally, the dry cell is packaged by an aluminum shell.
0.5 wt% FEC and 0.5 wt% VC additive, including electrolyte LiPF with concentration of 1.0mol/L6And injecting 30% of ethylene carbonate EC, 30% of ethyl methyl carbonate EMC and 40% of dimethyl carbonate DMC mixed organic solvent into the battery shell, and sealing the liquid injection port after liquid injection.
Forming a battery cell in a step-type charging mode, charging a battery to a specified voltage at a constant current of 0.1C, and then charging to a constant voltage of the specified voltage until the current is less than 0.02C; the cell was then discharged to the cut-off voltage at 0.1C, completing one cycle. Three charge-discharge cycles at 0.1,0.2,0.5C were performed in the range of 2.5-4.3V.
Tests prove that the specific energy of the aluminum-shell cylindrical battery prepared in the way is more than 280Wh/kg (0.2C), and the capacity retention rate is more than 80% after 500 cycles. And (3) after the battery is fully charged, the battery is placed in a low-temperature box at the temperature of-25 ℃ for 8 hours and is discharged in the environment, and the discharge capacity is not lower than 80% of the rated capacity.
Example 2:
97 wt% of modified LiNi0.905Co0.07Al0.02Mg0.005O20.75 wt% of conductive carbon black, 0.75 wt% of vapor grown carbon fiber and 1.5 wt% of PVDF were dissolved in NMP, respectively, to prepare positive electrode slurry.
89.2 wt% of modified graphite/4.8 wt% of silica mixed material, 1.5 wt% of conductive carbon black, 1.5 wt% of carbon nano tube, 1.5 wt% of CMC and 1.5 wt% of SBR were respectively dissolved in ultrapure water to prepare negative electrode slurry.
The positive electrode slurry is uniformly coated on the surface of an aluminum foil with the thickness of 12 mu m, and the density of double surfaces is 42mg/cm2The compacted density after one-time rolling is 3.5g/cm3(ii) a The cathode slurry is uniformly coated on the surface of a copper foil with the thickness of 8 mu m, and the density of two surfaces is 22mg/cm2The compacted density after one-time rolling is 1.3g/cm3。
Cutting the positive and negative electrode plates, winding into electric core, and coating Al with thickness of 16 μm between the positive and negative electrodes2O3The coating diaphragm is separated, the anode and cathode tabs of the anode and the cathode are wrapped by the cathode in the auxiliary material area and are fixed by welding, and finally, the dry cell is packaged by an aluminum shell.
0.5 wt% FEC and 0.5 wt% VC additive, including electrolyte LiPF with concentration of 1.0mol/L6The electrolyte of 30 percent of ethylene carbonate EC, 30 percent of ethyl methyl carbonate EMC and 40 percent of dimethyl carbonate DMC mixed organic solvent by volume fraction is injected into the battery shellAnd sealing the liquid injection port after liquid injection.
Forming a battery cell in a step-type charging mode, charging a battery to a specified voltage at a constant current of 0.1C, and then charging to a constant voltage of the specified voltage until the current is less than 0.02C; the cell was then discharged to the cut-off voltage at 0.1C, completing one cycle. Three charge-discharge cycles at 0.1,0.2,0.5C were performed in the range of 2.5-4.3V.
Tests prove that the specific energy of the aluminum-shell cylindrical battery prepared in the way is more than 290Wh/kg (0.2C), and the capacity retention rate is more than 80% after the cycle times are 400 times. And (3) after the battery is fully charged, the battery is placed in a low-temperature box at the temperature of-25 ℃ for 8 hours and is discharged in the environment, and the discharge capacity is not lower than 80% of the rated capacity.
In summary, the present invention can provide a high specific energy cylindrical lithium ion battery with high specific energy, high safety, long cycle life and excellent low-temperature discharge performance, and a method for preparing the same.
The present invention has been described in detail with reference to the above examples, but the description is only for the preferred examples of the present invention and should not be construed as limiting the scope of the present invention. All equivalent changes and modifications made within the scope of the present invention shall fall within the scope of the present invention.
Claims (8)
1. A high specific energy cylindrical lithium ion battery is characterized in that: the cylindrical lithium ion battery with high specific energy comprises a positive electrode material, a negative electrode material, electrolyte and a diaphragm,
the positive electrode material comprises 94-98% of active substance, 1-3% of conductive agent and 1-3% of polyvinylidene fluoride by mass fraction, the active substance is Mg-doped modified high-nickel NCA material, the conductive agent comprises conductive carbon black SP and vapor phase growth carbon fiber VGCF, and the mass ratio of the conductive carbon black SP to the vapor phase growth carbon fiber VGCF is MSP:MVGCF＝0.5-2；
The negative electrode material comprises 88-94% of active substance, 2-6% of conductive agent, 1-3% of sodium carboxymethyl cellulose (CMC), 1-3% of Styrene Butadiene Rubber (SBR), and 92-96% of modified graphite and 4-8% of silicon oxideThe graphite is modified by coating an amorphous carbon layer with the thickness of several nanometers on the surface, and the conductive agent comprises Carbon Nano Tubes (CNT) and conductive carbon black (SP) with the mass ratio of MSP:MCNT＝0.5-2；
The electrolyte comprises electrolyte LiPF with the concentration of 0.8-1.3mol/L6The paint comprises ethylene carbonate EC accounting for 20-40% of the solvent volume fraction, ethyl methyl carbonate EMC accounting for 20-40%, dimethyl carbonate DMC mixed organic solvent accounting for 20-40% of the solvent volume fraction, and a film forming additive;
the battery diaphragm is a coating diaphragm taking polyethylene terephthalate (PET) as a substrate, and the coating comprises SiO2、Al2O3Or poly (p-phenylene/m-phenylene terephthalamide).
2. The high specific energy cylindrical lithium ion battery of claim 1, wherein: the current collector used for the positive electrode is an aluminum foil with the thickness of 10-20 mu m, and the negative electrode is a copper foil with the thickness of 6-10 mu m; the density of the double-sided coating surface of the positive electrode is 40-46mg/cm2The density of the double-sided coating surface of the negative electrode is 20-24mg/cm2(ii) a The compacted density of the anode material is 3.4-3.8g/cm3The compacted density of the negative electrode material is 0.8-1.5g/cm3。
3. The high specific energy cylindrical lithium ion battery of claim 1, wherein: the positive active substance is Mg-doped and surface oxide-coated high-nickel NCA material LiNi0.91-xCo0.07Al0.02MgxO2Wherein the Mg mole fraction x is 0.005-0.02, the LiNi0.91-xCo0.07Al0.02MgxO2Has a particle diameter of 12-15 μm and a specific surface area of 0.4-0.6m2/g。
4. The high specific energy cylindrical lithium ion battery of claim 1, wherein: the value of the anode-cathode capacity ratio N/P of the electrode material is 1.0-2.0.
5. According to claim1 the high specific energy cylindrical lithium ion battery is characterized in that: the particle diameter d50 of the negative active material is 10-20 μm, and the specific surface area is 1-2m2/g。
6. The high specific energy cylindrical lithium ion battery of claim 1, wherein: the viscosity of the positive electrode slurry and the negative electrode slurry is 1500-6000 mPa.S, and the battery electrolyte film-forming additive is one or two of FEC and VC.
7. The high specific energy cylindrical lithium ion battery of claim 1, wherein: the battery shell is a steel shell or an aluminum shell.
8. A method for preparing a high specific energy lithium ion battery is characterized in that: the method for preparing the high specific energy lithium ion battery comprises the following steps:
the method comprises the following steps: mixing a positive active substance, a conductive agent and a binder into slurry by taking NMP as a solvent, uniformly coating the slurry on the surface of an aluminum foil, and drying, rolling and slitting the slurry to prepare a pole piece;
step two: mixing a negative electrode active substance, a conductive agent and a binder into slurry by taking ultrapure water as a solvent, uniformly coating the slurry on the surface of copper foil, and drying, rolling and slitting the slurry to prepare a pole piece;
step three: preparing the prepared positive plate, the prepared negative plate and the diaphragm into a battery cell in a winding mode, ensuring that a negative electrode in the material attachment area wraps a positive electrode, fixing tabs of the positive electrode and the negative electrode by welding, and finally packaging into a dry battery cell; injecting a certain amount of electrolyte into the battery cell; and (3) forming the battery cell to obtain the cylindrical lithium ion battery with high specific energy.
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