CN114497490B - Positive electrode slurry and preparation method thereof, battery cell group and preparation method thereof, and lithium battery - Google Patents
Positive electrode slurry and preparation method thereof, battery cell group and preparation method thereof, and lithium battery Download PDFInfo
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- CN114497490B CN114497490B CN202210041185.5A CN202210041185A CN114497490B CN 114497490 B CN114497490 B CN 114497490B CN 202210041185 A CN202210041185 A CN 202210041185A CN 114497490 B CN114497490 B CN 114497490B
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- 239000011267 electrode slurry Substances 0.000 title claims abstract description 125
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 58
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 58
- 238000002360 preparation method Methods 0.000 title claims abstract description 32
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 110
- 239000000843 powder Substances 0.000 claims abstract description 87
- 239000000741 silica gel Substances 0.000 claims abstract description 74
- 229910002027 silica gel Inorganic materials 0.000 claims abstract description 74
- 239000002904 solvent Substances 0.000 claims abstract description 23
- 239000006258 conductive agent Substances 0.000 claims abstract description 21
- 239000011230 binding agent Substances 0.000 claims abstract description 17
- 238000009987 spinning Methods 0.000 claims description 186
- 239000007774 positive electrode material Substances 0.000 claims description 63
- 239000000758 substrate Substances 0.000 claims description 50
- 238000002156 mixing Methods 0.000 claims description 25
- 238000010041 electrostatic spinning Methods 0.000 claims description 24
- 239000011248 coating agent Substances 0.000 claims description 22
- 238000000576 coating method Methods 0.000 claims description 22
- 238000001035 drying Methods 0.000 claims description 19
- 239000000463 material Substances 0.000 claims description 18
- 238000000034 method Methods 0.000 claims description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 14
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical group CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 claims description 14
- 239000002033 PVDF binder Substances 0.000 claims description 13
- -1 polytetrafluoroethylene Polymers 0.000 claims description 13
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 13
- 239000006229 carbon black Substances 0.000 claims description 12
- 239000002041 carbon nanotube Substances 0.000 claims description 12
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 12
- 239000003273 ketjen black Substances 0.000 claims description 10
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 9
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 9
- 239000002210 silicon-based material Substances 0.000 claims description 9
- 239000002002 slurry Substances 0.000 claims description 8
- 239000011206 ternary composite Substances 0.000 claims description 7
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 6
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 6
- 239000004917 carbon fiber Substances 0.000 claims description 6
- 229910021392 nanocarbon Inorganic materials 0.000 claims description 6
- 239000003960 organic solvent Substances 0.000 claims description 6
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 6
- 239000006256 anode slurry Substances 0.000 claims description 5
- 238000000227 grinding Methods 0.000 claims description 5
- 229920000459 Nitrile rubber Polymers 0.000 claims description 4
- KFDQGLPGKXUTMZ-UHFFFAOYSA-N [Mn].[Co].[Ni] Chemical compound [Mn].[Co].[Ni] KFDQGLPGKXUTMZ-UHFFFAOYSA-N 0.000 claims description 4
- 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 description 4
- 239000001768 carboxy methyl cellulose Substances 0.000 claims description 4
- 238000004519 manufacturing process Methods 0.000 claims description 4
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 claims description 4
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 claims description 4
- 229920003048 styrene butadiene rubber Polymers 0.000 claims description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 2
- 239000013543 active substance Substances 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 45
- 239000012528 membrane Substances 0.000 description 34
- 229910052751 metal Inorganic materials 0.000 description 30
- 239000002184 metal Substances 0.000 description 30
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 27
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 26
- 229910001416 lithium ion Inorganic materials 0.000 description 26
- 239000010410 layer Substances 0.000 description 22
- 238000009831 deintercalation Methods 0.000 description 21
- 239000000377 silicon dioxide Substances 0.000 description 18
- 238000001354 calcination Methods 0.000 description 17
- 239000011259 mixed solution Substances 0.000 description 16
- 150000001868 cobalt Chemical class 0.000 description 14
- 150000002696 manganese Chemical class 0.000 description 14
- 239000000203 mixture Substances 0.000 description 14
- 150000002815 nickel Chemical class 0.000 description 14
- 150000003681 vanadium Chemical class 0.000 description 14
- 239000003792 electrolyte Substances 0.000 description 13
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 12
- 239000011247 coating layer Substances 0.000 description 12
- 238000009830 intercalation Methods 0.000 description 12
- 230000002687 intercalation Effects 0.000 description 12
- 229910003002 lithium salt Inorganic materials 0.000 description 12
- 159000000002 lithium salts Chemical class 0.000 description 12
- 230000014759 maintenance of location Effects 0.000 description 12
- 239000006185 dispersion Substances 0.000 description 11
- 238000010438 heat treatment Methods 0.000 description 11
- 238000003825 pressing Methods 0.000 description 11
- 238000007581 slurry coating method Methods 0.000 description 11
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 10
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 10
- 229910052782 aluminium Inorganic materials 0.000 description 10
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 10
- 239000011889 copper foil Substances 0.000 description 10
- 239000011888 foil Substances 0.000 description 10
- 239000011148 porous material Substances 0.000 description 10
- 238000005096 rolling process Methods 0.000 description 10
- 239000011777 magnesium Substances 0.000 description 9
- 239000003381 stabilizer Substances 0.000 description 9
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 8
- 229910013716 LiNi Inorganic materials 0.000 description 8
- 239000000853 adhesive Substances 0.000 description 8
- 230000001070 adhesive effect Effects 0.000 description 8
- 230000008595 infiltration Effects 0.000 description 8
- 238000001764 infiltration Methods 0.000 description 8
- 239000011572 manganese Substances 0.000 description 8
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 7
- 229920002678 cellulose Polymers 0.000 description 7
- 239000001913 cellulose Substances 0.000 description 7
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 239000000839 emulsion Substances 0.000 description 6
- IIPYXGDZVMZOAP-UHFFFAOYSA-N lithium nitrate Chemical compound [Li+].[O-][N+]([O-])=O IIPYXGDZVMZOAP-UHFFFAOYSA-N 0.000 description 6
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical group [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 5
- AZFUOHYXCLYSQJ-UHFFFAOYSA-N [V+5].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O Chemical compound [V+5].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O AZFUOHYXCLYSQJ-UHFFFAOYSA-N 0.000 description 5
- 229910052786 argon Inorganic materials 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- 238000001816 cooling Methods 0.000 description 5
- 230000002349 favourable effect Effects 0.000 description 5
- 238000003475 lamination Methods 0.000 description 5
- 238000003756 stirring Methods 0.000 description 5
- 229910052720 vanadium Inorganic materials 0.000 description 5
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 5
- 238000004804 winding Methods 0.000 description 5
- 239000004721 Polyphenylene oxide Substances 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 229920000570 polyether Polymers 0.000 description 4
- 229920005862 polyol Polymers 0.000 description 4
- 229920001289 polyvinyl ether Polymers 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- 238000004064 recycling Methods 0.000 description 4
- 235000012239 silicon dioxide Nutrition 0.000 description 4
- 239000004094 surface-active agent Substances 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 description 3
- 229910001981 cobalt nitrate Inorganic materials 0.000 description 3
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 description 3
- 239000007773 negative electrode material Substances 0.000 description 3
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 description 3
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- 239000012752 auxiliary agent Substances 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 238000001514 detection method Methods 0.000 description 2
- 239000007772 electrode material Substances 0.000 description 2
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Chemical compound [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 description 2
- 238000009740 moulding (composite fabrication) Methods 0.000 description 2
- 150000007524 organic acids Chemical class 0.000 description 2
- 238000011056 performance test Methods 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 238000002791 soaking Methods 0.000 description 2
- INZDTEICWPZYJM-UHFFFAOYSA-N 1-(chloromethyl)-4-[4-(chloromethyl)phenyl]benzene Chemical compound C1=CC(CCl)=CC=C1C1=CC=C(CCl)C=C1 INZDTEICWPZYJM-UHFFFAOYSA-N 0.000 description 1
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000001419 dependent effect Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 238000009736 wetting Methods 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
-
- 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
- H01M4/364—Composites as mixtures
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Composite Materials (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Secondary Cells (AREA)
Abstract
The application provides positive electrode slurry and a preparation method thereof, a battery cell group and a preparation method thereof, and a lithium battery. The positive electrode slurry comprises a positive electrode active substance, a conductive agent, a binder, a solvent and nano silica gel powder, wherein the mass percentage of the nano silica gel powder is as followsThe positive electrode slurry can improve the charge-discharge multiplying power and the cycle performance of the lithium battery.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to positive electrode slurry and a preparation method thereof, a battery cell group and a preparation method thereof, and a lithium battery.
Background
The lithium battery has the advantages of high energy density, low self-discharge, good cycle stability and the like, is one of the most attractive energy storage devices at present, and the electrochemical performance of the lithium battery is greatly dependent on the selection of electrode materials and diaphragms, especially the selection of the electrode materials, wherein the positive electrode material requires the lithium ions to have a larger diffusion coefficient so as to facilitate the rapid charge and discharge of the lithium battery, namely the charge and discharge multiplying power of the lithium battery is ensured, and the structure of the positive electrode material is required not to be changed greatly in the deintercalation and intercalation processes of the lithium ions so as to ensure the cycle performance of the lithium battery, but the common lithium battery still has the problems of poor cycle performance and charge and discharge multiplying power.
Disclosure of Invention
The invention aims to overcome the defects in the prior art and provides positive electrode slurry capable of improving the charge-discharge multiplying power and the cycle performance of a lithium battery, a preparation method of the positive electrode slurry, a battery cell group, a preparation method of the battery cell group and the lithium battery.
The aim of the invention is realized by the following technical scheme:
the positive electrode slurry comprises a positive electrode active material, a conductive agent, a binder, a solvent and nano silica gel powder, wherein the mass percentage of the nano silica gel powder is as follows
In one embodiment, the positive electrode active material is a nickel cobalt manganese ternary composite positive electrode material.
In one embodiment, the conductive agent is at least one of carbon black, ketjen black, carbon fibers, and carbon nanotubes.
In one embodiment, the binder is at least one of polyvinylidene fluoride, polytetrafluoroethylene, polyvinyl alcohol, styrene-butadiene rubber, sodium carboxymethyl cellulose, nitrile rubber, and silica gel.
In one embodiment, the solvent is N-methylpyrrolidone.
A method for preparing a positive electrode slurry according to any one of the above embodiments, the method comprising the steps of:
Mixing and grinding the nano silica gel powder and the positive electrode active material to obtain a mixed material;
and uniformly mixing the conductive agent, the binder, the solvent and the mixed material to obtain the anode slurry.
The battery cell group comprises a positive plate, a diaphragm and a negative plate which are sequentially stacked, wherein the positive plate comprises a positive substrate and the positive slurry coated on the positive substrate, the diaphragm contains silica gel powder, and the negative plate comprises a negative substrate and the negative slurry coated on the negative substrate and containing a silicon-based material.
In one embodiment, the surface of the positive electrode substrate is coated with nanocarbon, and the nanocarbon layer is sandwiched between the positive electrode substrate and the positive electrode slurry.
A preparation method of a battery cell group is used for preparing the battery cell group in any embodiment, and the preparation method of the battery cell group comprises the following steps:
obtaining a positive electrode substrate and a negative electrode substrate;
carrying out positive electrode coating operation on the positive electrode base material by adopting positive electrode slurry, and then carrying out positive electrode drying treatment to obtain a positive electrode plate;
performing negative electrode coating operation on the negative electrode base material by adopting negative electrode slurry, and then performing negative electrode drying treatment to obtain a negative electrode plate;
Obtaining a diaphragm spinning solution containing silica gel powder;
carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate;
carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate;
carrying out bonding treatment on one side surface of the spinning positive plate containing spinning or/and one side surface of the spinning negative plate containing spinning;
and carrying out pressing treatment on the spinning positive plate and the spinning negative plate after the bonding treatment so as to combine the spinning positive plate and the spinning negative plate together to obtain the battery cell group.
A lithium battery comprising the battery cell stack of any of the above embodiments.
Compared with the prior art, the invention has at least the following advantages:
the positive electrode slurry comprises the following components in percentage by massAfter being mixed with the positive electrode active material, the nano silica gel powder is matched with the conductive agent, so that the conductivity of the positive electrode slurry is effectively improved, the intercalation and deintercalation of lithium ions are facilitated, the charge-discharge multiplying power of a lithium battery is further improved, and the rapid infiltration of the positive electrode slurry is facilitated; in addition, the mass percentage is as followsThe nano silica gel powder can offset the thermal expansion of the nano silica gel powder by utilizing the higher porosity of the nano silica gel powder and the porosity of the positive electrode active material, and can also play a supporting role on the positive electrode slurry, so that the collapse of the positive electrode slurry during the lithium ion deintercalation is reduced, and the cycle performance of a lithium battery is further improved.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings that are needed in the embodiments will be briefly described below, it being understood that the following drawings only illustrate some embodiments of the present invention and therefore should not be considered as limiting the scope, and other related drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a flow chart of a method for preparing a positive electrode slurry according to an embodiment of the present invention;
fig. 2 is a flowchart of a method for manufacturing a battery cell according to an embodiment of the invention.
Detailed Description
In order that the invention may be readily understood, a more complete description of the invention will be rendered by reference to the appended drawings. The drawings illustrate preferred embodiments of the invention. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete.
It will be understood that when an element is referred to as being "fixed to" another element, it can be directly on the other element or intervening elements may also be present. When an element is referred to as being "connected" to another element, it can be directly connected to the other element or intervening elements may also be present. The terms "vertical," "horizontal," "left," "right," and the like are used herein for illustrative purposes only and are not meant to be the only embodiment.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used herein in the description of the invention is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. The term "and/or" as used herein includes any and all combinations of one or more of the associated listed items.
The application provides a positive electrode slurry. The positive electrode slurry comprises a positive electrode active material, a conductive agent and a binderThe adhesive, the solvent and the nano silica gel powder, wherein the mass percentage of the nano silica gel powder is as follows
The positive electrode slurry comprises the following components in percentage by massAfter being mixed with the positive electrode active material, the nano silica gel powder is matched with the conductive agent, so that the conductivity of the positive electrode slurry is effectively improved, the intercalation and deintercalation of lithium ions are facilitated, the charge-discharge multiplying power of a lithium battery is further improved, and the rapid infiltration of the positive electrode slurry is facilitated; in addition, the mass percentage is as followsThe nano silica gel powder can offset the thermal expansion of the nano silica gel powder by utilizing the higher porosity of the nano silica gel powder and the porosity of the positive electrode active material, and can also play a supporting role on the positive electrode slurry, so that the collapse of the positive electrode slurry during the lithium ion deintercalation is reduced, and the cycle performance of a lithium battery is further improved.
In one embodiment, the conductive agent is at least one of carbon black, ketjen black, carbon fibers, and carbon nanotubes. It can be understood that carbon black, ketjen black, carbon fibers and carbon nanotubes can better form points, lines and surface-type lithium ion transfer and provide more binding sites for lithium ions, which is favorable for the deintercalation and intercalation of lithium ions, and further improves the charge and discharge multiplying power of lithium batteries.
In one embodiment, the binder is at least one of polyvinylidene fluoride, polytetrafluoroethylene, polyvinyl alcohol, styrene-butadiene rubber, sodium carboxymethyl cellulose, nitrile rubber, and silica gel. It is understood that at least one of polyvinylidene fluoride, polytetrafluoroethylene, polyvinyl alcohol, styrene-butadiene rubber, sodium carboxymethyl cellulose, nitrile rubber and silica gel is used as a binder of the positive electrode slurry, ensuring the adhesive strength of the positive electrode slurry on the positive electrode substrate.
In one embodiment, the solvent is N-methylpyrrolidone. It can be understood that N-methylpyrrolidone has a good compatibility with the positive electrode active material in the positive electrode slurry, and is easily removed when the positive electrode sheet is dried, and the stability of the positive electrode slurry is well ensured.
In one embodiment, the positive electrode active material is a nickel cobalt manganese ternary composite positive electrode material. It can be appreciated that the nickel-cobalt-manganese ternary composite positive electrode material and the methodThe nano silica gel powder is matched with the electrolyte to ensure that the positive electrode slurry has better electrolyte retention capacity and ensures that the positive electrode slurry has better charge-discharge multiplying power and cycle performance.
In one embodiment, the positive electrode active material is LiNi 1/3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/3 O 2-2y F y Wherein x is more than 0 and less than or equal to 0.01,0, and y is more than or equal to 0.05. It can be understood that the positive electrode active material is LiNi 1/3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/ 3 O 2-2y F y Has better stratum-shaped structure and electrochemical performance, and when used in positive electrode slurry, the composite material is matched withThe nano silica gel powder is matched, so that the structural stability of the layered structure of the positive electrode slurry coating layer on the surface of the positive electrode substrate is better ensured in the process of lithium ion deintercalation and intercalation, namely, collapse of the positive electrode slurry in the process of lithium ion deintercalation is reduced, the damage of the layered structure caused by expansion of the positive electrode slurry coating layer on the surface of the positive electrode substrate is reduced, and the cycle performance of the lithium battery is further improved.
It can be understood that the nano silica gel powder is nano silica, and the thermal expansion of the silica is lower than that of the silicon-based negative electrode material, but the positive electrode slurry coating layer on the surface of the positive electrode substrate is thinner, and even if the thermal expansion coefficient of the silica is lower, if the positive electrode slurry contains more silica, specifically, when the silicon content is more than 0.5 wt%, the positive electrode slurry is still expanded and contracted in the charging and discharging process of the lithium battery to affect the positive electrode Structural stability of the coating layer of the positive electrode slurry on the surface of the substrate, therefore, in the present application, in order to ensure the electrolyte retention capability of the positive electrode slurry and the wetting effect and the conductivity of the positive electrode slurry, a scheme of adopting silicon dioxide is reserved, and the usage amount of silicon dioxide is optimized from the whole formulation of the positive electrode slurry, in particular, it is found that in the case of using the ternary composite positive electrode active material doped with magnesium and vanadium metal, the usage amount of silicon dioxide is as followsAnd in addition, the collapse of the positive electrode slurry during the deintercalation of lithium ions is reduced, and the cycle performance, the charge-discharge multiplying power and the capacity retention rate of the lithium battery are further improved.
In one embodiment, x=0.01; y=0.05. It can be understood that when the positive electrode active material LiNi 1/ 3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/3 O 2-2y F y When x=0.01 and y=0.05, the positive electrode active material has a stable layered structure and good electrochemical performance, and further the cycle performance, the charge-discharge multiplying power and the capacity retention rate of the lithium battery are better ensured.
In one embodiment, the method for preparing the positive electrode active material includes the steps of:
placing lithium salt, nickel salt, cobalt salt, manganese salt, vanadium salt and organic acid into deionized water for mixing and dissolving operation to obtain a metal mixed solution;
heating the metal mixed solution to obtain metal sol;
calcining the metal sol;
and crushing the calcined metal sol to obtain the positive electrode active material.
According to the preparation method of the positive electrode active material, the lithium salt, the nickel salt, the cobalt salt, the manganese salt and the vanadium salt are dissolved by adopting the organic acid, so that the lithium salt, the nickel salt, the cobalt salt, the manganese salt and the vanadium salt are fully mixed and dissolved, the mixing uniformity of the lithium salt, the nickel salt, the cobalt salt, the manganese salt and the vanadium salt is further ensured, the heating operation of a metal mixed solution is further ensured, the dispersion uniformity of each material in the positive electrode active material obtained after the calcination treatment is further ensured, the stability of the layered structure of the formed positive electrode active material and the excellent electrochemical performance are further ensured, and the electrochemical performance and the cycle performance of a lithium battery are further improved.
In one embodiment, the method for preparing the positive electrode active material includes the steps of:
Placing lithium nitrate, nickel nitrate, cobalt nitrate, manganese nitrate, vanadium nitrate and citric acid into deionized water for mixing and dissolving operation to obtain a metal mixed solution;
heating the metal mixed solution to obtain metal sol;
calcining the metal sol;
and crushing the calcined metal sol to obtain the positive electrode active material.
According to the preparation method of the positive electrode active material, the nitrogen dioxide and the water are removed after the nitric acid is heated and calcined, so that the positive electrode slurry is prepared by adopting lithium nitrate, nickel nitrate, cobalt nitrate, manganese nitrate and vanadium nitrate, the introduction of impurity ions is reduced, the formation stability of a layered structure of the positive electrode active material is ensured, and the citric acid is utilized to mix and dissolve the lithium nitrate, nickel nitrate, cobalt nitrate, manganese nitrate and vanadium nitrate.
In one embodiment, the pH of the metal mixture solution is between 0.8 and 1.2. It can be understood that the PH of the metal mixed solution has a great influence on the electrochemical performance of the positive electrode active material, in particular, the stability of the cycle performance and the charge-discharge capacity retention rate of the lithium battery having the positive electrode active material, and it is difficult to ensure that the good cycle performance and the capacity retention rate are maintained at the same time in the case of a higher or lower PH, so that in the present application, the PH of the metal mixed solution is 0.8 to 1.2, so that the lithium battery having the positive electrode active material has the good cycle performance stability and the good charge-discharge capacity retention rate at the same time.
In one embodiment, the PH of the metal mixed solution is 1.0, which better ensures that the lithium battery with the positive electrode active material has better cycle performance stability and charge-discharge capacity retention rate.
In one embodiment, the molar ratio of the sum of nickel salt, cobalt salt, manganese salt and vanadium salt to lithium salt is 1: (1.2-1.6). It can be understood that when the molar ratio of the sum of the nickel salt, cobalt salt, manganese salt and vanadium salt to the lithium salt is 5/6 to 5/8, it is advantageous to form a positive electrode active material having better lithium ion deintercalation and intercalation ability, thereby better ensuring the first discharge specific capacity and cycle performance of the lithium battery.
In one embodiment, the molar ratio of the sum of the nickel salt, cobalt salt, manganese salt, and vanadium salt to the lithium salt is 1:1.5. It can be understood that when the molar ratio of the sum of the nickel salt, cobalt salt, manganese salt and vanadium salt to the lithium salt is 1:1.5, the formed positive electrode active material is better ensured to have better lithium ion deintercalation and intercalation capability, and further, the first charge-discharge specific capacity and the cycle performance of the lithium battery are better ensured.
In one embodiment, the molar ratio of nickel salt, cobalt salt, manganese salt, and vanadium salt is 0.1:0.2:0.4:0.2. It can be understood that when the molar ratio of the nickel salt, the cobalt salt, the manganese salt and the vanadium salt is 0.1:0.2:0.4:0.2, the discharge specific capacity of the positive electrode slurry reaches 200mAh/g, and the stable generation of the positive electrode active material with a better layered structure and electrochemical performance is facilitated.
In one embodiment, the molar ratio of the sum of nickel salt, cobalt salt, manganese salt, vanadium salt and lithium salt to citric acid is 1.8 to 2.5. It can be understood that when the content of citric acid is higher, the groups in the citric acid interfere with the internal structure of the active material, so that the layered structure of the generated positive electrode active material is disordered and the internal groups are aggregated, namely, the structure of the positive electrode active material is in a disordered state, so that the specific discharge capacity and the cycle stability of a lithium battery using the positive electrode slurry are reduced, therefore, in the application, the molar ratio of the sum of nickel salt, cobalt salt, manganese salt, vanadium salt and lithium salt to the citric acid is 1.8-2.5, the stable and ordered layered structure of the positive electrode active material is better ensured, and the specific discharge capacity and the cycle stability of the lithium battery containing the positive electrode slurry are further ensured.
In one embodiment, the molar ratio of the sum of the nickel salt, cobalt salt, manganese salt, vanadium salt and lithium salt to citric acid is 2. It can be understood that the molar ratio of the sum of the nickel salt, cobalt salt, manganese salt, vanadium salt and lithium salt to citric acid is 2, so that the stable and ordered layered structure of the positive electrode active material is better ensured, and the specific discharge capacity and the cycling stability of the lithium battery containing the positive electrode slurry are further ensured.
In one embodiment, the heating operation is performed on the metal mixed solution at a temperature of 80 to 90 ℃. It can be understood that the purpose of the heating operation of the metal mixed solution is to reduce the content of the solvent in the metal mixed solution, which is advantageous for the calcination of the metal mixed solution, and the heating of the metal mixed solution at 80-90 ℃ is advantageous for ensuring the orderly stabilization of the layered structure of the positive electrode active material formed after the calcination.
In one embodiment, the metal sol is calcined, which specifically includes the following steps: pre-calcining the metal sol;
carrying out secondary calcination treatment on the pre-calcined metal sol;
and (3) performing three times of calcination treatment on the metal sol subjected to the secondary calcination treatment.
The metal sol is calcined, and contains citric acid and vanadium nitrate, namely, the metal sol is provided with a carbon source, when the vanadium nitrate is calcined, high-valence oxides of the vanadium sublimate and are consumed at a lower temperature, and then a three-stage calcining mode is needed, so that the oxidation valence of the vanadium is kept at a lower temperature, and then the temperature is increased to continue calcining, thereby being beneficial to promoting the stable generation of the vanadium-doped ternary composite material.
In one embodiment, the pre-calcination treatment is performed on the metal sol at a temperature of 400-500 ℃ for 2-3 hours. It can be understood that calcination is carried out at 400-500 ℃ for 2-3 hours, thereby effectively ensuring the rapid removal of the solvent and ensuring the stability of each substance in the metal sol.
In one embodiment, the temperature of the secondary calcination treatment of the pre-calcined metal sol is 600-700 ℃ and the time is 3-5 h. It can be understood that calcination is continued at 600-700 ℃ for 3-5 hours, effectively ensuring the reduction of the valence of the high valence oxide of vanadium and effectively ensuring the stable generation of the ternary composite material doped with vanadium.
In one embodiment, the temperature of the third calcination treatment is 800-1350 ℃ and the time is 6-8 hours. It can be understood that the calcination is continued at 800-1350 ℃ for 6-8 hours, thereby effectively ensuring the stable generation of the positive electrode active material with better layered structure and electrochemical performance.
The application also provides a preparation method of the positive electrode slurry, which is used for preparing the positive electrode slurry of any embodiment. The preparation method of the positive electrode slurry comprises the following steps: mixing and grinding the nano silica gel powder and the positive electrode active material to obtain a mixed material; and uniformly mixing the conductive agent, the binder, the solvent and the mixed material to obtain the anode slurry.
According to the preparation method of the positive electrode slurry, after the nano silica gel powder is fully dispersed in the pores of the positive electrode active material, the nano silica gel powder is mixed with the conductive agent, the binder and the solvent, so that the nano silica gel powder is fully filled in the pores of the positive electrode active material, the deintercalation and intercalation capacity of lithium ions in the positive electrode slurry is better improved, the collapse of a positive electrode slurry coating layer on the surface of a positive electrode substrate during the deintercalation of the lithium ions is reduced, and the cycle performance and the charge-discharge multiplying power of a lithium battery containing the positive electrode slurry are further improved.
If the nano silica gel powder, the positive electrode active material, the conductive agent, the binder and the solvent are directly mixed or ground, the nano silica gel powder is difficult to fully fill in the positive electrode active material, and the nano silica gel powder is easy to agglomerate and disperse unevenly, so that the problem of collapse of the positive electrode slurry coating layer on the surface of the positive electrode substrate when the nano silica gel powder is matched with the positive electrode active material to alleviate lithium ion deintercalation is difficult to be realized.
Referring to fig. 2, in order to better understand the preparation method of the positive electrode slurry of the present application, the preparation method of the positive electrode slurry of the present application is further explained below, and the preparation method of the positive electrode slurry of an embodiment includes the following steps:
St100, carrying out mixed grinding operation on the nano silica gel powder and the positive electrode active material to obtain a mixed material. It can be understood that, because the content of the nano silica gel powder is smaller, and the particle size of the nano silica gel powder is smaller, agglomeration easily occurs in water or a gas solvent, in order to better match the nano silica gel powder with the positive electrode active material and increase the deintercalation and intercalation capability of lithium ions in the positive electrode slurry, and better match the positive electrode active material and reduce the collapse of the positive electrode slurry coating layer on the surface of the positive electrode substrate when the lithium ions are deintercalated, firstly, the nano silica gel powder and the positive electrode active material are subjected to grinding operation, so that the nano silica gel powder is fully filled in the pores of the positive electrode active material, the deintercalation and intercalation capability of lithium ions in the positive electrode slurry is better improved, and the collapse of the positive electrode slurry coating layer on the surface of the positive electrode substrate when the lithium ions are deintercalated is reduced, and further the cycle performance and the charge-discharge multiplying power of the lithium battery containing the positive electrode slurry are improved.
St200, uniformly mixing the conductive agent, the binder, the solvent and the mixed material to obtain the positive electrode slurry. It can be understood that after the nano silica gel powder is fully dispersed in the pores of the positive electrode active material, the nano silica gel powder is mixed with the conductive agent, the binder and the solvent, so that the full dispersion of the nano silica gel powder is effectively ensured, and the nano silica gel powder is effectively ensured to be matched with the positive electrode active material, thereby achieving the purpose of reducing the collapse of the positive electrode slurry coating layer on the surface of the positive electrode substrate during the deintercalation of lithium ions.
According to the preparation method of the positive electrode slurry, after the nano silica gel powder is fully dispersed in the pores of the positive electrode active material, the nano silica gel powder is mixed with the conductive agent, the binder and the solvent, so that the nano silica gel powder is fully filled in the pores of the positive electrode active material, the deintercalation and intercalation capacity of lithium ions in the positive electrode slurry is better improved, the collapse of a positive electrode slurry coating layer on the surface of a positive electrode substrate during the deintercalation of the lithium ions is reduced, and the cycle performance and the charge-discharge multiplying power of a lithium battery containing the positive electrode slurry are further improved.
The application also provides a battery cell group. The battery cell group comprises a positive plate, a diaphragm and a negative plate which are sequentially stacked, wherein the positive plate comprises a positive substrate and the positive slurry coated on the positive substrate, the diaphragm contains silica gel powder, and the negative plate comprises a negative substrate and the negative slurry coated on the negative substrate and containing a silicon-based material.
The battery cell group comprises the nano silica gel powder in the positive electrode slurry, the silica gel powder in the diaphragm, and the silicon-based material in the negative electrode slurry, so that the battery cell group can be effectively soaked by electrolyte, the electrolyte retaining capacity of the battery cell group is ensured, and even when the positive electrode plate, the diaphragm and the negative electrode plate in the battery cell group are tightly laminated and attached, the soaking of the battery cell group can still be better ensured, the full embodiment of the performance of the battery cell group is ensured, and the electrochemical performance and the recycling service life of the battery cell group are ensured.
In one embodiment, the surface of the positive electrode substrate is coated with nano carbon, and the nano carbon layer is clamped between the positive electrode substrate and the positive electrode slurry, so that the electrochemical performance and the cycle performance of the battery cell group are improved.
In one embodiment, the negative electrode slurry includes lithium titanate, lithium fluoride, vanadium carbide, a silicon-based material, a graphite negative electrode material, a binder, a conductive agent, and a solvent. It can be understood that the positive electrode slurry and the diaphragm contain silicon dioxide, and the negative electrode slurry contains silicon-based materials, namely the positive electrode slurry, the diaphragm and the negative electrode material contain silicon-based materials, so that the positive electrode plate, the diaphragm and the negative electrode plate have good wettability, the integrated battery cell group has good wettability, namely the uniform stability of the battery cell group is ensured, the performance of the battery cell group is fully reflected, and the electrochemical performance and the recycling service life of the battery cell group are ensured.
In one embodiment, the conductive agent of the negative electrode slurry is the same as the conductive agent of the positive electrode slurry, ensuring the conductivity of the negative electrode slurry.
In one embodiment, the solvent of the negative electrode slurry comprises hydrofluoric acid and an organic solvent, so that the dispersion uniformity of the negative electrode slurry is ensured, and the electrochemical performance and the cycle performance of the battery cell group are further ensured.
The application also provides a preparation method of the battery cell group, which is used for preparing the battery cell group in any embodiment. The preparation method of the battery cell group comprises the following steps: obtaining a positive electrode substrate and a negative electrode substrate; carrying out positive electrode coating operation on a positive electrode base material by adopting positive electrode slurry, and then carrying out positive electrode drying treatment to obtain a positive electrode plate; performing negative electrode coating operation on a negative electrode base material by adopting negative electrode slurry, and then performing negative electrode drying treatment to obtain a negative electrode plate; obtaining a diaphragm spinning solution containing silica gel powder; carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate; carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate; carrying out adhesive treatment on one side surface of the spinning positive plate containing spinning or/and one side surface of the spinning negative plate containing spinning; and (3) carrying out press fit treatment on the spinning positive plate and the spinning negative plate after the bonding treatment so as to combine the spinning positive plate and the spinning negative plate together to obtain the battery cell group.
According to the preparation method of the battery cell group, the diaphragms are integrally spun and formed on the positive plate and the negative plate respectively, and the spun positive plate and the spun negative plate are combined together, so that the stability of the layer structure of the battery cell group is ensured, and the quick lamination or winding and forming of the battery cell group are facilitated; in addition, the membrane with more pores and containing silica gel powder is favorable for the electrolyte to infiltrate the battery cell group, and is favorable for the electrolyte to enter the positive plate and the negative plate to infiltrate the positive plate and the negative plate, so that the infiltration uniformity of the battery cell group is ensured, and the electrochemical performance and the cycle performance of the battery cell group are improved.
In order to better understand the preparation method of the battery cell set of the present application, the preparation method of the battery cell set of the present application is further explained below, and the preparation method of the battery cell set of an embodiment includes the following steps:
s100, obtaining a positive electrode substrate and a negative electrode substrate. It can be understood that the electrochemical performance of the battery cell group depends on the performance of the positive electrode and the negative electrode to a good degree, so as to better realize the charge-discharge multiplying power, the battery capacity retention rate and the cycle performance of the battery cell group, the positive electrode slurry and the negative electrode slurry are generally adjusted based on the positive electrode substrate and the negative electrode substrate, so that the improvement of the electrochemical performance of the battery cell group is most effectively realized, but the difficulty of improving the performance of the battery cell group is greater by further adjusting the positive electrode slurry and the negative electrode slurry, so that in the application, the difficulty of improving the performance of the battery cell group is reduced by matching the structure of the battery cell group with the components of the battery cell group, namely, the structure and the components are adjusted based on the positive electrode substrate and the negative electrode substrate, and the performance of the battery cell group is improved.
And S200, carrying out positive electrode coating operation on the positive electrode base material by adopting positive electrode slurry, and then carrying out positive electrode drying treatment to obtain the positive electrode plate. It can be appreciated that the preparation of the positive electrode sheet containing the silica gel powder is achieved by coating the positive electrode slurry on the positive electrode substrate.
And S300, carrying out negative electrode coating operation on a negative electrode base material by adopting negative electrode slurry, and then carrying out negative electrode drying treatment to obtain a negative electrode plate. It can be appreciated that the preparation of the negative electrode sheet containing the silicon-based material is realized by coating the negative electrode slurry on the negative electrode substrate.
S400, obtaining the diaphragm spinning solution containing the silica gel powder. It can be understood that the membrane spinning solution containing the silica gel powder can realize electrostatic spinning of the membrane so as to form a membrane with more pores and containing the silica gel powder, the more pores and containing the silica gel powder are beneficial to infiltration of electrolyte, and electrolyte enters the positive plate and the negative plate to infiltrate the positive plate and the negative plate, so that infiltration uniformity of the battery cell group is ensured, and electrochemical performance and cycle performance of the battery cell group are improved.
S500, carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate. It can be understood that the membrane spinning solution is used for electrostatic spinning to form a membrane, and the anode plate is subjected to anode electrostatic spinning operation, namely, the electrostatic spinning is performed on the anode slurry coating layer on the surface of the anode substrate, namely, the membrane and the anode plate are integrated, so that the problem of inaccurate alignment of the membrane and the anode plate is solved, and the rapid lamination or winding forming of the battery cell group is facilitated.
And S600, carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate. It can be understood that the membrane spinning solution is used for electrostatic spinning to form a membrane, and the anode plate is subjected to anode electrostatic spinning operation, namely, electrostatic spinning is performed on the anode slurry coating layer on the surface of the anode substrate, namely, the membrane and the anode plate are formed into a whole, so that the problem of inaccurate alignment of the membrane and the anode plate is solved, and the rapid lamination or winding forming of the battery cell group is facilitated; in addition, the diaphragm spinning solution is directly subjected to electrostatic spinning on the negative electrode plate to form a diaphragm, so that the diaphragm has an acting force for preventing cracking on the negative electrode slurry on the negative electrode substrate, the stability of the layer structure of the battery cell group is improved, and the cycle performance and the capacity retention rate of the lithium battery are further improved.
And S700, carrying out bonding treatment on one side surface of the spinning positive plate containing spinning or/and one side surface of the spinning negative plate containing spinning. It can be understood that the spinning positive plate and the spinning negative plate can be bonded by one side surface containing spinning or/and one side surface containing spinning, so that the bonding of the spinning positive plate and the spinning negative plate is realized, namely, the integration of the positive plate, the diaphragm and the negative plate of the battery cell group is realized, and the diaphragm is respectively and directly integrated on the positive slurry layer and the negative slurry layer, thereby being beneficial to the rapid lamination or winding forming of the battery cell group.
And S800, performing press fit treatment on the spinning positive plate and the spinning negative plate after the bonding treatment so as to combine the spinning positive plate and the spinning negative plate together to obtain the battery cell group. It can be understood that the side surface of the spinning positive plate containing the spinning or/and the side surface of the spinning negative plate containing the spinning is subjected to bonding treatment, and then the bonding treatment is performed on the spinning positive plate and the spinning negative plate after the bonding treatment, so that the bonding stability of the battery core is effectively ensured.
According to the preparation method of the battery cell group, the diaphragms are integrally spun and formed on the positive plate and the negative plate respectively, and the spun positive plate and the spun negative plate are combined together, so that the stability of the layer structure of the battery cell group is ensured, and the quick lamination or winding and forming of the battery cell group are facilitated; in addition, the membrane with more pores and containing silica gel powder is favorable for the electrolyte to infiltrate the battery cell group, and is favorable for the electrolyte to enter the positive plate and the negative plate to infiltrate the positive plate and the negative plate, so that the infiltration uniformity of the battery cell group is ensured, and the electrochemical performance and the cycle performance of the battery cell group are improved.
In one embodiment, the method for obtaining the membrane spinning solution containing the silica gel powder specifically comprises the following steps: and performing dispersion operation on cellulose, nano alumina powder, an adhesive, an auxiliary agent, a stabilizer, a surfactant and a solvent to obtain the diaphragm spinning solution. It can be understood that the self-discharge of the diaphragm containing cellulose, nano alumina powder adhesive, auxiliary agent, stabilizer, surfactant and solvent is low, the diaphragm has better infiltration liquid-retaining capacity and higher toughness, and the probability of the diaphragm being pierced or punctured is further reduced; in addition, the battery pack has good high temperature resistance, and can not shrink, deform or melt under the condition of increasing the charge and discharge temperature of the battery, so that the short circuit problem of the battery pack is reduced, and the use safety of the battery pack is effectively ensured.
In one embodiment, the membrane spinning solution comprises the following components in parts by mass: 95 to 120 parts of cellulose, 10 to 30 parts of nano alumina powder, 5 to 10 parts of adhesive, 0.1 to 2 parts of stabilizer, 0.2 to 1 part of surfactant and 50 to 65 parts of solvent.
In one embodiment, the bonding treatment of the side surface of the spun positive electrode sheet containing the spinning or/and the side surface of the spun negative electrode sheet containing the spinning is specifically: and (3) adopting an organic solvent to erode one side surface of the spinning positive plate containing spinning or/and one side surface of the spinning negative plate containing spinning so as to enable the one side surface of the spinning positive plate containing spinning or/and one side surface of the spinning negative plate containing spinning to form a solution layer. It can be understood that the spinning positive plate contains a side surface of spinning or/and the spinning negative plate contains a side surface of spinning solution layer, namely, a solution layer in a dissolved state is formed on the membrane spinning on the positive plate and/or a solution layer in a dissolved state is formed on the membrane spinning on the negative plate, so that the combination of the membrane spinning on the positive plate and the membrane spinning on the negative plate is facilitated, the combination strength of the membrane spinning on the positive plate and the membrane spinning on the negative plate is facilitated, the structural stability of the battery cell group is further facilitated, and the stability of the lithium battery is further improved.
In one embodiment, the bonding-treated spun positive plate and the bonding-treated spun negative plate are subjected to pressing treatment, so that the spun positive plate and the spun negative plate are combined together specifically as follows: and (3) abutting and pressing the solution layer of the spinning positive plate and one side surface of the spinning negative plate containing spinning so as to combine the spinning positive plate and the spinning negative plate together. It can be understood that the solution layer of the spinning positive plate and the spinning negative plate are pressed against one side surface containing spinning, namely molecules of the solution layer on the spinning positive plate and spinning on the spinning negative plate are mixed, namely compatibility on molecules occurs between membrane spinning on the spinning positive plate and membrane spinning on the spinning negative plate, so that the bonding strength of the spinning positive plate and the spinning negative plate is enhanced, the structural stability of the battery cell group is effectively improved, and the stability of the lithium battery is further improved.
In one embodiment, the bonding-treated spun positive plate and the bonding-treated spun negative plate are subjected to pressing treatment, so that the spun positive plate and the spun negative plate are combined together specifically as follows: and (3) pressing one side surface of the spinning positive plate containing spinning against the solution layer of the spinning negative plate so as to combine the spinning positive plate and the spinning negative plate together. It can be understood that the spinning positive plate is pressed against the solution layer of the spinning negative plate by one side surface containing spinning, so that molecules of the solution layer on the spinning negative plate and spinning on the spinning positive plate are mixed, namely, compatibility on molecules occurs between membrane spinning on the spinning positive plate and membrane spinning on the spinning negative plate, and further, the bonding strength of the spinning positive plate and the spinning negative plate is enhanced, the structural stability of the battery cell group is effectively improved, and the stability of the lithium battery is further improved.
In one embodiment, the bonding-treated spun positive plate and the bonding-treated spun negative plate are subjected to pressing treatment, so that the spun positive plate and the spun negative plate are combined together specifically as follows: the solution layer of the spinning positive plate and the solution layer of the spinning negative plate are pressed against each other, so that the spinning positive plate and the spinning negative plate are combined together, the solution layer on the spinning positive plate and the solution layer on the spinning negative plate are better compatible in molecules, the bonding strength of the spinning positive plate and the spinning negative plate is further enhanced, the structural stability of the battery cell group is effectively improved, and the stability of the lithium battery is further improved.
In one embodiment, the binder in the membrane dope comprises polytetrafluoroethylene emulsion and/or polyvinylidene fluoride emulsion, ensuring the adhesion stability of the membrane.
In one embodiment, the organic solvent is a volatile organic solvent, so that the membrane is effectively eroded to form a solution layer, and then the compatibility of the membrane on the surface of the positive electrode plate and the membrane on the surface of the negative electrode plate is realized, namely the compatibility between molecules of the membrane on the surface of the positive electrode plate and the membrane on the surface of the negative electrode plate is realized, and further the structural stability of the battery cell group is effectively improved.
In one embodiment, the organic solvent comprises ethanol and/or methanol, so that the compatibility between molecules of the membrane on the surface of the positive electrode plate and the membrane on the surface of the negative electrode plate is better realized, and the structural stability of the cell group is further effectively improved.
In one embodiment, the surfactant is a tertiary alkyl polyol polyvinyl ether and/or polyether modified silicone.
In one embodiment, the stabilizer is a silicate stabilizer. In one embodiment, after the step of laminating the spun positive electrode sheet and the spun negative electrode sheet after the bondable treatment, the method for manufacturing the cell stack further includes the steps of: and drying the spun positive plate and the spun negative plate after the pressing treatment.
The application also provides a lithium battery. The lithium battery comprises the battery cell group of any embodiment. In this embodiment, the battery cell group includes positive electrode sheet, diaphragm and negative electrode sheet that stacks gradually, and the positive electrode sheet includes positive electrode substrate and the positive electrode thick liquids of any one of the above-mentioned embodiments of coating on positive electrode substrate, and the diaphragm contains silica gel powder, and the negative electrode sheet includes negative electrode substrate and the negative electrode thick liquids of coating on negative electrode substrate.
According to the lithium battery, the battery cell group is used, the nano silica gel powder is contained in the positive electrode slurry of the battery cell group, the silica gel powder is contained in the diaphragm, and the silicon-based material is contained in the negative electrode slurry, so that the battery cell group can be effectively soaked by electrolyte, the electrolyte retaining capacity of the battery cell group is ensured, and even when the positive electrode plate, the diaphragm and the negative electrode plate in the battery cell group are tightly laminated and attached, the soaking of the battery cell group can still be better ensured, the full embodiment of the performance of the battery cell group is ensured, the electrochemical performance and the recycling service life of the battery cell group are ensured, namely the electrochemical performance and the recycling service life of the lithium battery are ensured.
Compared with the prior art, the invention has at least the following advantages:
the positive electrode slurry comprises the following components in percentage by massAfter being mixed with the positive electrode active material, the nano silica gel powder is matched with the conductive agent, so that the conductivity of the positive electrode slurry is effectively improved, the intercalation and deintercalation of lithium ions are facilitated, the charge-discharge multiplying power of a lithium battery is further improved, and the rapid infiltration of the positive electrode slurry is facilitated; in addition, the mass percentage is as followsThe nano silica gel powder can offset the thermal expansion of the nano silica gel powder by utilizing the higher porosity of the nano silica gel powder and the porosity of the positive electrode active material, and can also support the positive electrode slurryThe method reduces collapse of the positive electrode slurry during lithium ion deintercalation, and improves cycle performance of the lithium battery.
The following examples are given in detail, and it should be noted that they are not exhaustive of all possible scenarios, and that the materials used in the following examples are available commercially unless otherwise specified.
Example 1
Obtaining a copper foil and an aluminum foil;
mixing 0.004kg of nano silica gel powder with 7kg of LiNi 1/3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/3 O 2-2y F y (x=0.01; y=0.05), then adding 0.1kg of a mixture of ketjen black and carbon nanotubes, 0.5kg of polyvinylidene fluoride and a proper amount of N-methyl pyrrolidone, and stirring and mixing to obtain positive electrode slurry;
Coating the positive electrode slurry on an aluminum foil sheet, and then, carrying out rolling drying to obtain a positive electrode sheet;
taking 5kg of silica powder, carrying out heat treatment for 2 hours at 900 ℃ under the protection of argon, cooling to room temperature, and then adding 0.1kg of a mixture of ketjen black and carbon nano tubes, 0.5kg of polyvinylidene fluoride and a proper amount of a mixed solution of N-methylpyrrolidone and hydrofluoric acid into the heat-treated silica powder for dispersion and mixing to obtain negative electrode slurry;
coating the negative electrode slurry on a copper foil, and then, carrying out rolling drying to obtain a negative electrode plate;
dispersing 9.5kg of cellulose, 1kg of nano alumina powder, 0.5g of polytetrafluoroethylene emulsion, 0.01kg of silicate stabilizer, 0.02kg of tertiary alkyl polyol polyvinyl ether and 5kg of ethanol to obtain a diaphragm spinning solution;
carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate;
carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate;
carrying out adhesive treatment on the side surface of the spinning positive plate containing the spinning;
and (3) carrying out pressing treatment on the spinning positive plate and the spinning negative plate after the bonding treatment so as to combine the spinning positive plate and the spinning negative plate together to obtain a battery cell group, and then assembling and forming the battery cell group to obtain the lithium battery.
Example 2
Obtaining a copper foil and an aluminum foil;
mixing 0.008kg of nano silica gel powder with 7kg of LiNi 1/3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/3 O 2-2y F y (x=0.01; y=0.05), then adding 0.1kg of a mixture of carbon black and carbon fiber, 0.5kg of polytetrafluoroethylene and a proper amount of N-methylpyrrolidone, and stirring and mixing to obtain positive electrode slurry;
coating the positive electrode slurry on an aluminum foil sheet, and then, carrying out rolling drying to obtain a positive electrode sheet;
taking 5kg of silica powder, carrying out heat treatment for 2 hours at 900 ℃ under the protection of argon, cooling to room temperature, and then adding 0.1kg of a mixture of carbon black and carbon fibers, 0.5kg of polytetrafluoroethylene and a proper amount of a mixed solution of N-methylpyrrolidone and hydrofluoric acid into the heat-treated silica powder for dispersion and mixing to obtain negative electrode slurry;
coating the negative electrode slurry on a copper foil, and then, carrying out rolling drying to obtain a negative electrode plate;
10kg of cellulose, 1.5kg of nano alumina powder, 0.6kg of polytetrafluoroethylene emulsion, 0.05kg of silicate stabilizer, 0.05kg of polyether modified organosilicon and 5.5kg of ethanol are subjected to dispersion operation to obtain a diaphragm spinning solution;
carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate;
carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate;
Carrying out adhesive treatment on the side surface of the spinning negative plate containing spinning;
and (3) carrying out pressing treatment on the spinning positive plate and the spinning negative plate after the bonding treatment so as to combine the spinning positive plate and the spinning negative plate together to obtain a battery cell group, and then assembling and forming the battery cell group to obtain the lithium battery.
Example 3
Obtaining a copper foil and an aluminum foil;
mixing 0.015kg of nano silica gel powder with 7kg of LiNi 1/3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/3 O 2-2y F y (x=0.01; y=0.02), then adding 0.1kg of a mixture of carbon black and carbon nanotubes, 0.5kg of polyvinyl alcohol and a proper amount of N-methylpyrrolidone, and stirring and mixing to obtain positive electrode slurry;
coating the positive electrode slurry on an aluminum foil sheet, and then, carrying out rolling drying to obtain a positive electrode sheet;
taking 5kg of silica powder, carrying out heat treatment at 1000 ℃ for 2 hours under the protection of argon, cooling to room temperature, and then adding 0.1kg of a mixture of carbon black and carbon nano tubes, 0.5kg of polyvinyl alcohol and a proper amount of a mixed solution of N-methylpyrrolidone and hydrofluoric acid into the heat-treated silica powder for dispersion and mixing to obtain negative electrode slurry;
coating the negative electrode slurry on a copper foil, and then, carrying out rolling drying to obtain a negative electrode plate;
10kg of cellulose, 2kg of nano alumina powder, 0.8kg of polyvinylidene fluoride emulsion, 0.1kg of silicate stabilizer, 0.08kg of mixture of tertiary alkyl polyol polyvinyl ether and polyether modified organosilicon and 6kg of methanol are subjected to dispersion operation to obtain a diaphragm spinning solution;
Carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate;
carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate;
carrying out bonding treatment on one side surface of the spinning positive plate containing spinning and one side surface of the spinning negative plate containing spinning;
and (3) carrying out pressing treatment on the spinning positive plate and the spinning negative plate after the bonding treatment so as to combine the spinning positive plate and the spinning negative plate together to obtain a battery cell group, and then assembling and forming the battery cell group to obtain the lithium battery.
Example 4
Obtaining a copper foil and an aluminum foil;
mixing 0.023kg of nano silica gel powder with 7kg of LiNi 1/3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/3 O 2-2y F y (x=0.01; y=0.03), then adding 0.1kg of carbon black, a mixture of carbon nanotubes and ketjen black, 0.5kg of polyvinylidene fluoride and a proper amount of N-methyl pyrrolidone, and stirring and mixing to obtain positive electrode slurry;
coating the positive electrode slurry on an aluminum foil sheet, and then, carrying out rolling drying to obtain a positive electrode sheet;
taking 5kg of silica powder, carrying out heat treatment for 2 hours at 1000 ℃ under the protection of argon, cooling to room temperature, and then adding 0.1kg of carbon black, a mixture of carbon nano tubes and ketjen black, 0.5kg of polyvinylidene fluoride and a proper amount of mixed liquid of N-methylpyrrolidone and hydrofluoric acid into the heat-treated silica powder for dispersion and mixing to obtain negative electrode slurry;
Coating the negative electrode slurry on a copper foil, and then, carrying out rolling drying to obtain a negative electrode plate;
dispersing 12kg of cellulose, 3kg of nano alumina powder, 1kg of polyvinylidene fluoride emulsion, 0.2kg of silicate stabilizer, 0.1kg of mixture of tertiary alkyl polyol polyvinyl ether and polyether modified organosilicon and 6.5kg of ethanol to obtain a diaphragm spinning solution;
carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate;
carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate;
carrying out bonding treatment on one side surface of the spinning positive plate containing spinning and one side surface of the spinning negative plate containing spinning;
and (3) carrying out pressing treatment on the spinning positive plate and the spinning negative plate after the bonding treatment so as to combine the spinning positive plate and the spinning negative plate together to obtain a battery cell group, and then assembling and forming the battery cell group to obtain the lithium battery.
Comparative example 1
Obtaining a copper foil and an aluminum foil;
mixing 0.023kg of nano silica gel powder with 7kg of LiNi 1/3 Co 1/3-x/3 Mn 1/3-x/3 Mg x/3 V x/3 O 2-2y F y (x=0.01; y=0.05), then adding 0.1kg of carbon black, a mixture of carbon nanotubes and ketjen black, 0.5kg of polyvinylidene fluoride and a proper amount of N-methyl pyrrolidone, and stirring and mixing to obtain positive electrode slurry;
Coating the positive electrode slurry on an aluminum foil sheet, and then, carrying out rolling drying to obtain a positive electrode sheet;
taking 5kg of silica powder, carrying out heat treatment for 2 hours at 1000 ℃ under the protection of argon, cooling to room temperature, and then adding 0.1kg of carbon black, a mixture of carbon nano tubes and ketjen black, 0.5kg of polyvinylidene fluoride and a proper amount of mixed liquid of N-methylpyrrolidone and hydrofluoric acid into the heat-treated silica powder for dispersion and mixing to obtain negative electrode slurry;
coating the negative electrode slurry on a copper foil, and then, carrying out rolling drying to obtain a negative electrode plate;
and sequentially stacking the positive plate, the diaphragm and the negative plate to obtain a battery cell group, and then assembling and forming the battery cell group to obtain the lithium battery.
The lithium batteries obtained in examples 1 to 4 and comparative example 1 were subjected to constant current charge/discharge performance test on a battery test system (LanD CTR 2001A) in a voltage range of 0.01 to 1.5V, cycle performance of the lithium batteries was tested at 1000mA/g charge/discharge, and internal micro short circuit test was performed on the lithium batteries obtained in examples 1 to 4 and comparative example 1, and the test results were as follows (average values obtained after testing a plurality of sets of lithium batteries in each of the following uniform examples and comparative examples).
Table 1: performance test results of lithium battery
| Sample of | First charge and discharge efficiency (%) | Capacity retention of 100 cycles (%) | Internal resistance (mΩ) | Short circuit detection pass rate |
| Example 4 | 85 | 74 | 1.39 | 92％ |
| Example 1 | 82 | 79 | 1.40 | 90％ |
| Example 3 | 83 | 75 | 1.42 | 95％ |
| Example 2 | 86 | 83 | 1.32 | 98％ |
| Comparative example 1 | 80 | 67 | 1.58 | 84％ |
From table 1, it can be seen that the battery cell group of the application has better first charge and discharge efficiency, better circulation capacity retention rate, smaller internal resistance and higher short circuit detection passing rate, and the battery cell group of the application has better electrochemical performance.
The above examples illustrate only a few embodiments of the invention, which are described in detail and are not to be construed as limiting the scope of the invention. It should be noted that it will be apparent to those skilled in the art that several variations and modifications can be made without departing from the spirit of the invention, which are all within the scope of the invention. Accordingly, the scope of protection of the present invention is to be determined by the appended claims.
Claims (6)
1. The preparation method of the battery cell group is characterized by comprising the following steps:
obtaining a positive electrode substrate and a negative electrode substrate;
carrying out positive electrode coating operation on the positive electrode base material by adopting positive electrode slurry, and then carrying out positive electrode drying treatment to obtain a positive electrode plate;
Performing negative electrode coating operation on the negative electrode base material by adopting negative electrode slurry, and then performing negative electrode drying treatment to obtain a negative electrode plate;
obtaining a diaphragm spinning solution containing silica gel powder;
carrying out positive electrode electrostatic spinning operation on the diaphragm spinning solution on the positive electrode plate to obtain a spinning positive electrode plate;
carrying out negative electrode electrostatic spinning operation on the diaphragm spinning solution on the negative electrode plate to obtain a spinning negative electrode plate;
adopting an organic solvent to erode one side surface of the spinning positive plate containing spinning or/and one side surface of the spinning negative plate containing spinning so as to enable the one side surface of the spinning positive plate containing spinning or/and one side surface of the spinning negative plate containing spinning to form a solution layer;
the solution layer of the spinning positive plate is pressed against one side surface of the spinning negative plate containing spinning so as to combine the spinning positive plate and the spinning negative plate together to obtain an electric core group;
the positive electrode slurry comprises a positive electrode active material, a conductive agent, a binder, a solvent and nano silica gel powder, wherein the mass percentage of the nano silica gel powder is 5- ‱ wt% -3 per mill wt;
the binder is at least one of polyvinylidene fluoride, polytetrafluoroethylene, polyvinyl alcohol, styrene-butadiene rubber, sodium carboxymethyl cellulose, nitrile rubber and silica gel;
The solvent is N-methyl pyrrolidone;
the preparation method of the positive electrode slurry comprises the following steps:
mixing and grinding the nano silica gel powder and the positive electrode active material to obtain a mixed material;
and uniformly mixing the conductive agent, the binder, the solvent and the mixed material to obtain the anode slurry.
2. The method for manufacturing a battery cell pack according to claim 1, wherein the positive electrode active material is a nickel-cobalt-manganese ternary composite positive electrode material.
3. The method of claim 1, wherein the conductive agent is at least one of carbon black, ketjen black, carbon fiber, and carbon nanotubes.
4. A battery cell group manufactured by the manufacturing method of the battery cell group according to any one of claims 1 to 3, wherein the battery cell group comprises a positive plate, a diaphragm and a negative plate which are sequentially stacked, the positive plate comprises a positive substrate and the positive slurry coated on the positive substrate, the diaphragm contains silica gel powder, and the negative plate comprises a negative substrate and the negative slurry coated on the negative substrate and containing a silicon-based material.
5. The battery pack of claim 4, wherein the surface of the positive electrode substrate is coated with nanocarbon, and the nanocarbon layer is sandwiched between the positive electrode substrate and positive electrode slurry.
6. A lithium battery comprising the cell stack of any one of claims 4-5.
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