CN113782705B - Positive plate of lithium ion battery, preparation method of positive plate and lithium ion battery - Google Patents
Positive plate of lithium ion battery, preparation method of positive plate and lithium ion battery Download PDFInfo
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- CN113782705B CN113782705B CN202111049051.XA CN202111049051A CN113782705B CN 113782705 B CN113782705 B CN 113782705B CN 202111049051 A CN202111049051 A CN 202111049051A CN 113782705 B CN113782705 B CN 113782705B
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 98
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 98
- 238000002360 preparation method Methods 0.000 title abstract description 22
- 239000000463 material Substances 0.000 claims abstract description 195
- 230000001502 supplementing effect Effects 0.000 claims abstract description 53
- 238000000034 method Methods 0.000 claims abstract description 20
- 239000007774 positive electrode material Substances 0.000 claims description 61
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 38
- 229910052799 carbon Inorganic materials 0.000 claims description 38
- 239000002033 PVDF binder Substances 0.000 claims description 35
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 35
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 25
- 239000011248 coating agent Substances 0.000 claims description 22
- 238000000576 coating method Methods 0.000 claims description 22
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 18
- 239000002245 particle Substances 0.000 claims description 12
- HFCVPDYCRZVZDF-UHFFFAOYSA-N [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O Chemical compound [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O HFCVPDYCRZVZDF-UHFFFAOYSA-N 0.000 claims description 10
- 239000013078 crystal Substances 0.000 claims description 6
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 claims description 5
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 claims description 5
- 230000000153 supplemental effect Effects 0.000 claims description 5
- 239000000126 substance Substances 0.000 claims description 4
- 229910013716 LiNi Inorganic materials 0.000 claims description 3
- 238000010030 laminating Methods 0.000 claims description 3
- 239000011572 manganese Substances 0.000 claims description 3
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 abstract description 35
- 229910052744 lithium Inorganic materials 0.000 abstract description 35
- 239000003792 electrolyte Substances 0.000 abstract description 17
- 239000011888 foil Substances 0.000 abstract description 14
- 238000004519 manufacturing process Methods 0.000 abstract description 14
- 238000007086 side reaction Methods 0.000 abstract description 13
- 238000003860 storage Methods 0.000 abstract description 12
- 238000005056 compaction Methods 0.000 abstract description 10
- 238000013461 design Methods 0.000 abstract description 7
- 230000009286 beneficial effect Effects 0.000 abstract description 6
- 230000007774 longterm Effects 0.000 abstract description 6
- 239000002904 solvent Substances 0.000 description 32
- 239000002002 slurry Substances 0.000 description 27
- OTYYBJNSLLBAGE-UHFFFAOYSA-N CN1C(CCC1)=O.[N] Chemical compound CN1C(CCC1)=O.[N] OTYYBJNSLLBAGE-UHFFFAOYSA-N 0.000 description 20
- 239000007789 gas Substances 0.000 description 17
- 238000003756 stirring Methods 0.000 description 16
- 230000000052 comparative effect Effects 0.000 description 15
- 229910015872 LiNi0.8Co0.1Mn0.1O2 Inorganic materials 0.000 description 11
- 238000002156 mixing Methods 0.000 description 11
- 239000006229 carbon black Substances 0.000 description 10
- 229910052782 aluminium Inorganic materials 0.000 description 8
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 7
- 238000001035 drying Methods 0.000 description 7
- 238000005520 cutting process Methods 0.000 description 6
- 230000007423 decrease Effects 0.000 description 6
- 238000005096 rolling process Methods 0.000 description 6
- 238000007605 air drying Methods 0.000 description 5
- 238000009775 high-speed stirring Methods 0.000 description 5
- 239000006185 dispersion Substances 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 150000001875 compounds Chemical class 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 239000011149 active material Substances 0.000 description 2
- 239000000853 adhesive Substances 0.000 description 2
- 230000001070 adhesive effect Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 238000004132 cross linking Methods 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 230000018109 developmental process Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 229910052814 silicon oxide Inorganic materials 0.000 description 2
- 239000013589 supplement Substances 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 239000006258 conductive agent Substances 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 230000002542 deteriorative effect Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000011267 electrode slurry Substances 0.000 description 1
- 239000007770 graphite material Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 1
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 description 1
- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000008719 thickening Effects 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention provides a positive plate of a lithium ion battery, a preparation method of the positive plate and the lithium ion battery. According to the invention, the prepared lithium ion battery can obtain high compaction and low direct current resistance, meanwhile, the side reaction of the battery is reduced, and the long-term circulation and storage stability of the battery are improved, which is beneficial to the three-layer structure design of the dressing layer, so that on one hand, the direct contact of lithium supplementing materials with electrolyte is reduced, and the gas production in the subsequent process of the battery is reduced; on the other hand, the contact surface between the whole dressing layer and the foil is optimized, the direct current resistance of the battery is reduced, the internal resistance of the battery is comprehensively improved, and the stability of the battery is improved.
Description
Technical Field
The invention belongs to the technical field of lithium ion battery development, relates to a design of a positive plate, and particularly relates to a positive plate of a lithium ion battery, a preparation method of the positive plate and the lithium ion battery.
Background
Silicon oxide composite graphite materials (C-SiOx) are used in high energy density power cell systems because of their relatively high theoretical specific capacities (> 400 mAh/g) and relatively low reaction potentials (< 0.4V). Is widely studied at presentLithium ion supplementary material Li 5 FeO 4 The (LFO) has higher first-time charging capacity (> 700 mAh/g) and lower first-time coulombic efficiency (< 10%), and good lithium ion supplementing effect.
In LFO materials, the oxidation level of some lattice oxygen is around 4.2V for lithium potential. Thus, oxygen is released during the first charge. The released oxygen reacts with the electrolyte to break the stable CEI film between the positive electrode and the electrolyte, thereby deteriorating the stability of the battery and even causing safety problems. Therefore, development and design of a positive electrode sheet of a lithium battery are needed to improve the defects of the prior art.
Disclosure of Invention
Aiming at the defects existing in the prior art, the invention aims to provide a positive plate of a lithium ion battery, a preparation method thereof and the lithium ion battery, and in the invention, the prepared lithium ion battery can obtain high compaction and low direct current resistance, meanwhile, the side reaction of the battery is reduced, the long-term circulation and storage stability of the battery are improved, and the double-layer structure design of a dressing layer is beneficial, so that on one hand, the direct contact of a lithium supplementing material with electrolyte is reduced, and the gas production in the subsequent process of the battery is reduced; on the other hand, the contact surface between the whole dressing layer and the foil is optimized, the direct current resistance of the battery is reduced, the internal resistance of the battery is comprehensively improved, and the stability of the battery is improved.
To achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the invention provides a positive plate of a lithium ion battery, the positive plate comprises a pole plate body, a dressing layer is arranged on the surface of the pole plate body, the dressing layer comprises a first material layer and a second material layer which are sequentially stacked along the surface of the pole plate body, and the mass ratio of lithium ion supplementing material to positive material in the first material layer is different from that of lithium ion supplementing material to positive material in the second material layer.
According to the invention, the prepared lithium ion battery can obtain high compaction and low direct current resistance, meanwhile, the side reaction of the battery is reduced, and the long-term circulation and storage stability of the battery are improved, which is beneficial to the double-layer structure design of the dressing layer, so that on one hand, the direct contact of lithium supplementing materials with electrolyte is reduced, and the gas production in the subsequent process of the battery is reduced; on the other hand, the contact surface between the whole dressing layer and the foil is optimized, the direct current resistance of the battery is reduced, the internal resistance of the battery is comprehensively improved, and the stability of the battery is improved.
As a preferable technical scheme of the invention, the mass ratio of the lithium ion supplementary material to the positive electrode material in the first material layer is larger than that of the lithium ion supplementary material to the positive electrode material in the second material layer.
The invention particularly limits that the mass ratio of the lithium ion supplementing material to the positive electrode material in the first material layer is larger than that of the lithium ion supplementing material to the positive electrode material in the second material layer, wherein the main reason is that the contact between the lithium ion supplementing material and the electrolyte is reduced, the side reaction is inhibited, and if the mass ratio of the lithium ion supplementing material to the positive electrode material in the first material layer is smaller than that of the lithium ion supplementing material to the positive electrode material in the second material layer, the lithium ion supplementing material and the electrolyte can generate severe side reaction, so that the gas production performance of storage is deteriorated.
Preferably, the first material layer includes a lithium ion supplemental material, a positive electrode material, conductive carbon black, conductive carbon tube, polyvinylidene fluoride, and a solvent.
Preferably, the mass ratio of the lithium ion supplementary material, the positive electrode material, the conductive carbon black, the conductive carbon tube, the polyvinylidene fluoride and the solvent in the first material layer is (1-5): (90-99): 1:0.5:40:1.
the invention is particularly limited in that the first material layer comprises lithium ion supplementary material, positive electrode material, conductive carbon black, conductive carbon tube, solvent and polyvinylidene fluoride in mass ratio of (1-5): (90-99): 1:0.5:40:1, wherein the main reason is that if any one of the components is absent or other components are added, the electrode sheet cannot be prepared, and thus a battery cannot be manufactured; and if the mass ratio exceeds the limit value, the electrode is difficult to manufacture, because the mass overrun has a large influence on the viscosity of the slurry.
Preferably, the thickness of the first material layer is 5 to 30 μm.
The thickness of the first material layer is particularly limited to 5-30 μm, and if the thickness exceeds the limit value by 30 μm, the direct current internal resistance (DCR) is increased, because the dressing layer is thickened, and lithium ions are difficult to diffuse; if the thickness thereof is less than the limit value of 5 μm, it may cause a decrease in the energy density of the battery due to a decrease in the amount of the lithium ion supplemental material added.
As a preferable technical scheme of the invention, the second material layer comprises a lithium ion supplementing material, a positive electrode material, conductive carbon black, conductive carbon tubes, polyvinylidene fluoride and a solvent.
Preferably, the mass ratio of the lithium ion supplementary material, the positive electrode material, the conductive carbon black, the conductive carbon tube, the polyvinylidene fluoride and the solvent in the second material layer is (0.1-1): (90-99): 1:0.5:40:1.
the invention is particularly limited in that the second material layer comprises lithium ion supplementary material, positive electrode material, conductive carbon black, conductive carbon tube, solvent and polyvinylidene fluoride in mass ratio of (0.1-1): (90-99): 1:0.5:40:1, wherein the main reason is that if any one of the components is absent or other components are added, the electrode sheet cannot be prepared, and thus a battery cannot be manufactured; and if the mass ratio exceeds the limit value, the electrode is difficult to manufacture, because the mass overrun has a large influence on the viscosity of the slurry.
Preferably, the thickness of the second material layer is 20-60 μm.
The thickness of the second material layer is particularly limited to 20-60 μm, and if the thickness exceeds the limit value of 60 μm, the direct current internal resistance (DCR) can be increased, because the dressing layer is thickened, and lithium ions are difficult to diffuse; if the thickness is less than the limit value of 20 μm, the stored gas yield increases because the first material layer is easily exposed to the electrolyte and side reactions continue to occur.
As a preferable technical scheme of the invention, the positive electrode material is nickel cobalt lithium manganate or lithium iron phosphate.
Preferably, the chemical formula of the nickel cobalt lithium manganate is LiNi x Co y Mn 1-x-y O 2 Wherein x is more than or equal to 0.5 and less than or equal to 0.9, and y is more than or equal to 0 and less than or equal to 0.2.
As a preferable technical scheme of the invention, the nickel cobalt lithium manganate is in a secondary spherical state or a single crystal state.
In a preferred embodiment of the present invention, the secondary lithium nickel cobalt manganese oxide spheres have a particle size of 9 to 25 μm, and may be, for example, 9 μm, 10 μm, 12 μm, 14 μm, 16 μm, 18 μm, 20 μm, 21 μm, 23 μm, or 25 μm, but are not limited to the listed values, and other values not listed in the range of values are equally applicable.
The particle size of the lithium nickel cobalt manganese oxide single crystal is preferably 2 to 6 μm, and may be, for example, 2 μm, 3 μm, 4 μm, 5 μm, or 6 μm, but is not limited to the listed values, and other values not listed in the range are equally applicable.
As a preferable technical scheme of the invention, the lithium iron phosphate is spherical lithium iron phosphate or nano lithium iron phosphate.
In a preferred embodiment of the present invention, the particle size of the spherical lithium iron phosphate is 6 to 15. Mu.m, for example, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 13 μm, 14 μm, 15 μm, but the present invention is not limited to the above-mentioned values, and other values not mentioned in the above-mentioned range are applicable.
The particle size of the nano lithium iron phosphate is preferably 0.3 to 2.0 μm, and may be, for example, 0.3 μm, 0.5 μm, 0.7 μm, 1.0 μm, 1.2 μm, 1.4 μm, 1.6 μm, 1.8 μm, 2.0 μm, but is not limited to the recited values, and other non-recited values within the range of the values are equally applicable.
In a second aspect, the present invention provides a method for preparing the positive electrode sheet according to the first aspect, where the method includes:
and sequentially laminating and coating a first material layer and a second material layer on the surface of the electrode plate body to form the positive electrode plate.
In a third aspect, the invention provides a lithium ion battery, which comprises a positive plate, a diaphragm and a negative plate which are sequentially stacked, wherein the positive plate is the positive plate in the first aspect.
Compared with the prior art, the invention has the beneficial effects that:
according to the invention, the prepared lithium ion battery can obtain high compaction and low direct current resistance, meanwhile, the side reaction of the battery is reduced, and the long-term circulation and storage stability of the battery are improved, which is beneficial to the double-layer structure design of the dressing layer, so that on one hand, the direct contact of lithium supplementing materials with electrolyte is reduced, and the gas production in the subsequent process of the battery is reduced; on the other hand, the contact surface between the whole dressing layer and the foil is optimized, the direct current resistance of the battery is reduced, the internal resistance of the battery is comprehensively improved, and the stability of the battery is improved.
Drawings
Fig. 1 is a schematic structural diagram of a positive plate of a lithium ion battery according to an embodiment of the present invention;
FIG. 2 is a graph showing the density of positive electrode sheets of lithium ion batteries according to example 1 and comparative example 1 of the present invention;
fig. 3 is a dc resistance diagram of the positive electrode sheet of the lithium ion battery provided in example 1 and comparative example 1 of the present invention;
fig. 4 is a graph showing the gassing results of the positive electrode sheets of lithium ion batteries according to the present invention provided in example 1 and comparative example 1.
Reference numerals: 1-a first material layer; 2-a second material layer; 3-aluminum foil.
Detailed Description
The technical scheme of the invention is further described below by the specific embodiments with reference to the accompanying drawings.
In the prior art, a technical scheme provides a positive plate of a lithium ion battery, which comprises a positive electrode current collector and a positive electrode active material layer coated on the positive electrode current collector, wherein the positive electrode active material layer contains a positive electrode active material, a conductive agent, a binder and a lithium-rich compound, and the lithium-rich compound generates lithium ions when the lithium ion battery is charged in a formation mode and releases one or more of gas, conductive carbon and a substance with electrochemical lithium storage activity.
Another technical scheme provides a lithium ion battery positive plate, which comprises a positive current collector, a conductive coating and an electrode layer; the positive current collector is a carbon film, the carbon film has a three-dimensional porous structure, and a conductive coating is arranged on the surface of the positive current collector; the conductive coating is of a double-layer structure and has a crosslinking gradient, and the crosslinking degree decreases from the second conductive coating to the first conductive coating; the electrode layer is wrapped on the surface of the second conductive coating; has the characteristics of excellent structural stability, heat resistance and good solvent resistance.
Another technical scheme provides a lithium ion battery positive plate and a preparation method thereof, wherein the lithium ion battery positive plate comprises a positive electrode material and an aluminum-based current collector, the positive electrode material comprises a positive electrode active material, a conductive material and a bonding material, and the bonding material is a composite water-soluble adhesive containing a water-soluble adhesive and a phosphate-containing compound.
However, the above technical solutions do not solve the problems that the lithium ion battery has high compaction and low direct current resistance, and meanwhile, the side reaction of the battery can be reduced, and the long-term cycle and storage stability of the battery are increased.
In order to solve at least the above technical problems, the present invention provides a positive plate of a lithium ion battery, as shown in fig. 1, where the positive plate includes a pole plate body, a dressing layer is disposed on a surface of the pole plate body, and the dressing layer includes a first material layer 1 and a second material layer 2 that are sequentially stacked along a surface of the pole plate body, and further, a mass ratio of a lithium ion supplementary material and a positive material in the first material layer 1 is different from a mass ratio of a lithium ion supplementary material and a positive material in the second material layer 2.
According to the invention, the prepared lithium ion battery can obtain high compaction and low direct current resistance, meanwhile, the side reaction of the battery is reduced, and the long-term circulation and storage stability of the battery are improved, which is beneficial to the double-layer structure design of the dressing layer, so that on one hand, the direct contact of lithium supplementing materials with electrolyte is reduced, and the gas production in the subsequent process of the battery is reduced; on the other hand, the contact surface between the whole dressing layer and the foil is optimized, the direct current resistance of the battery is reduced, the internal resistance of the battery is comprehensively improved, and the stability of the battery is improved.
The mass ratio of the lithium ion supplementary material to the positive electrode material in the first material layer 1 is greater than the mass ratio of the lithium ion supplementary material to the positive electrode material in the second material layer 2.
The invention particularly limits that the mass ratio of the lithium ion supplementing material to the positive electrode material in the first material layer is larger than that of the lithium ion supplementing material to the positive electrode material in the second material layer, wherein the main reason is that the contact between the lithium ion supplementing material and the electrolyte is reduced, the side reaction is inhibited, and if the mass ratio of the lithium ion supplementing material to the positive electrode material in the first material layer is smaller than that of the lithium ion supplementing material to the positive electrode material in the second material layer, the lithium ion supplementing material and the electrolyte can generate severe side reaction, so that the gas production performance of storage is deteriorated.
The first material layer 1 comprises a lithium ion supplementing material, a positive electrode material, conductive carbon black, conductive carbon tubes, polyvinylidene fluoride and a solvent, and further, the mass ratio of the lithium ion supplementing material to the positive electrode material to the conductive carbon black to the conductive carbon tubes to the polyvinylidene fluoride to the solvent is (1-5): (90-99): 1:0.5:40:1.
the invention is characterized in that the first material layer 1 comprises the following components in percentage by mass: (90-99): 1:0.5:40:1, the main reason is that if any one of the components is absent or other components are added, the electrode sheet cannot be prepared, and thus a battery cannot be manufactured; and if the mass ratio exceeds the limit value, the electrode is difficult to manufacture, because the mass overrun has a large influence on the viscosity of the slurry.
The thickness of the first material layer 1 is 5-30 μm, the invention particularly limits the thickness of the first material layer 1 to 5-30 μm, if the thickness exceeds the limit value of 30 μm, the direct current internal resistance (DCR) is increased, because the dressing layer is thickened, and lithium ions are difficult to diffuse; if the thickness thereof is less than the limit value of 5 μm, it may cause a decrease in the energy density of the battery due to a decrease in the amount of the lithium ion supplemental material added.
The second material layer 2 comprises a lithium ion supplementing material, a positive electrode material, conductive carbon black, conductive carbon tubes, polyvinylidene fluoride and a solvent, and further, the mass ratio of the lithium ion supplementing material to the positive electrode material to the conductive carbon black to the conductive carbon tubes to the polyvinylidene fluoride to the solvent is (0.1-1): (90-99): 1:0.5:40:1.
the invention is characterized in that the second material layer 2 comprises the following components in percentage by mass (0.1-1): (90-99): 1:0.5:40:1, wherein the main reason is that if any one of the components is absent or other components are added, the electrode sheet cannot be prepared, and thus a battery cannot be manufactured; and if the mass ratio exceeds the limit value, the electrode is difficult to manufacture, because the mass overrun has a large influence on the viscosity of the slurry.
The thickness of the second material layer 2 is 20-60 μm, the invention particularly limits the thickness of the second material layer 2 to 20-60 μm, if the thickness exceeds the limit value of 60 μm, the direct current internal resistance (DCR) can be increased, because the dressing layer is thickened, and lithium ions are difficult to diffuse; if the thickness is less than the limit value of 20 μm, the stored gas yield increases because the first material layer is easily exposed to the electrolyte and side reactions continue to occur.
The positive electrode material is nickel cobalt lithium manganate or lithium iron phosphate, and further, the chemical formula of the nickel cobalt lithium manganate is LiNi x Co y Mn 1-x-y O 2 Wherein x is more than or equal to 0.5 and less than or equal to 0.9, y is more than or equal to 0 and less than or equal to 0.2, and further, the nickel cobalt lithium manganate is in a secondary sphere form or a single crystal form, the particle size of the nickel cobalt lithium manganate in the secondary sphere form is 9-25 mu m, and the particle size of the nickel cobalt lithium manganate in the single crystal form is 2-6 mu m.
The lithium iron phosphate is spherical lithium iron phosphate or nano lithium iron phosphate, and further, the particle size of the spherical lithium iron phosphate is 6-15 mu m, and the particle size of the nano lithium iron phosphate is 0.3-2.0 mu m.
In one embodiment, the invention provides a preparation method of a positive plate, which comprises the following steps:
and sequentially laminating and coating a first material layer 1 and a second material layer 2 on the surface of the pole piece body to form the positive pole piece.
In another embodiment, the invention provides a lithium ion battery, which comprises a positive plate, a separator and a negative plate which are sequentially stacked, wherein the positive plate adopts the positive plate of the first aspect.
Example 1
The embodiment provides a preparation method of a positive plate of a lithium ion battery, wherein:
(1) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 3:99:1:0.5:40:1 to obtain a first material layer 1, wherein the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, preparing conductive slurry by high-speed dispersion and stirring for 2 hours, and preparing a first material layer 1 by high-speed stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry;
(2) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 0.5:99:1:0.5:40:1 to obtain a second material layer 2, and the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, dispersing and stirring for 2 hours at high speed to prepare conductive slurry, and then stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry at high speed to prepare a second material layer 2;
(3) Uniformly coating the prepared first material layer 1 and second material layer 2 on the aluminum foil 3 pole piece body by using a scraper in the sequence of the first material layer 1 and the second material layer 2, wherein the thickness of the first material layer 1 is 15 mu m, and the thickness of the second material layer 2 is 45 mu m;
(4) And (3) placing the pole piece body coated in the step (3) in a forced air drying oven, drying for 20min at 120 ℃, rolling and cutting the dried pole piece with the pressure of 20MPa to prepare a positive pole piece, and calculating the mass of the coating in unit volume at the moment to obtain the compacted density of the pole piece.
Example 2
The embodiment provides a preparation method of a positive plate of a lithium ion battery, wherein:
(1) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 1:99:1:0.5:40:1 to obtain a first material layer 1, wherein the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, preparing conductive slurry by high-speed dispersion and stirring for 2 hours, and preparing a first material layer 1 by high-speed stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry;
(2) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 0.1:99:1:0.5:40:1 to obtain a second material layer 2, and the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, dispersing and stirring for 2 hours at high speed to prepare conductive slurry, and then stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry at high speed to prepare a second material layer 2;
(3) Uniformly coating the prepared first material layer 1 and second material layer 2 on the aluminum foil 3 pole piece body by using a scraper in the sequence of the first material layer 1 and the second material layer 2, wherein the thickness of the first material layer 1 is 5 mu m, and the thickness of the second material layer 2 is 20 mu m;
(4) And (3) placing the pole piece body coated in the step (3) in a forced air drying oven, drying for 20min at 120 ℃, rolling and cutting the dried pole piece with the pressure of 20MPa to prepare a positive pole piece, and calculating the mass of the coating in unit volume at the moment to obtain the compacted density of the pole piece.
Example 3
The embodiment provides a preparation method of a positive plate of a lithium ion battery, wherein:
(1) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is as followsIs 2:99:1:0.5:40:1 to obtain a first material layer 1, wherein the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, preparing conductive slurry by high-speed dispersion and stirring for 2 hours, and preparing a first material layer 1 by high-speed stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry;
(2) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 0.3:99:1:0.5:40:1 to obtain a second material layer 2, and the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, dispersing and stirring for 2 hours at high speed to prepare conductive slurry, and then stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry at high speed to prepare a second material layer 2;
(3) Uniformly coating the prepared first material layer 1 and second material layer 2 on the aluminum foil 3 pole piece body by using a scraper in the sequence of the first material layer 1 and the second material layer 2, wherein the thickness of the first material layer 1 is 10 mu m, and the thickness of the second material layer 2 is 30 mu m;
(4) And (3) placing the pole piece body coated in the step (3) in a forced air drying oven, drying for 20min at 120 ℃, rolling and cutting the dried pole piece with the pressure of 20MPa to prepare a positive pole piece, and calculating the mass of the coating in unit volume at the moment to obtain the compacted density of the pole piece.
Example 4
The embodiment provides a preparation method of a positive plate of a lithium ion battery, wherein:
(1) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 4:99:1:0.5:40:1 to obtain a first material layer 1, wherein the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tube and azomethineThe mass ratio of the polyvinylpyrrolidone solvent to the polyvinylidene fluoride is 1:0.5:40:1, preparing conductive slurry by high-speed dispersion and stirring for 2 hours, and preparing a first material layer 1 by high-speed stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry;
(2) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 0.7:99:1:0.5:40:1 to obtain a second material layer 2, and the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, dispersing and stirring for 2 hours at high speed to prepare conductive slurry, and then stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry at high speed to prepare a second material layer 2;
(3) Uniformly coating the prepared first material layer 1 and second material layer 2 on the aluminum foil 3 pole piece body by using a scraper in the sequence of the first material layer 1 and the second material layer 2, wherein the thickness of the first material layer 1 is 20 mu m, and the thickness of the second material layer 2 is 50 mu m;
(4) And (3) placing the pole piece body coated in the step (3) in a forced air drying oven, drying for 20min at 120 ℃, rolling and cutting the dried pole piece with the pressure of 20MPa to prepare a positive pole piece, and calculating the mass of the coating in unit volume at the moment to obtain the compacted density of the pole piece.
Example 5
The embodiment provides a preparation method of a positive plate of a lithium ion battery, wherein:
(1) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 5:99:1:0.5:40:1 to obtain a first material layer 1, wherein the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1 high-speed dispersing and stirring for 2 hours to prepare conductive slurry, and then adding lithium supplementing material and positive electrode materialMixing with conductive slurry at high speed to prepare a first material layer 1;
(2) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) The mass ratio of the conductive carbon black, the conductive carbon tube, the nitrogen methyl pyrrolidone solvent and the polyvinylidene fluoride is 1:99:1:0.5:40:1 to obtain a second material layer 2, and the specific preparation method comprises the following steps: firstly, conducting carbon black, conducting carbon tubes, a nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride are mixed according to the mass ratio of 1:0.5:40:1, dispersing and stirring for 2 hours at high speed to prepare conductive slurry, and then stirring and mixing a lithium supplementing material, a positive electrode material and the conductive slurry at high speed to prepare a second material layer 2;
(3) Uniformly coating the prepared first material layer 1 and second material layer 2 on the aluminum foil 3 pole piece body by using a scraper in the sequence of the first material layer 1 and the second material layer 2, wherein the thickness of the first material layer 1 is 30 mu m, and the thickness of the second material layer 2 is 60 mu m;
(4) And (3) placing the pole piece body coated in the step (3) in a forced air drying oven, drying for 20min at 120 ℃, rolling and cutting the dried pole piece with the pressure of 20MPa to prepare a positive pole piece, and calculating the mass of the coating in unit volume at the moment to obtain the compacted density of the pole piece.
Example 6
The present example provides a method for preparing a positive electrode sheet of a lithium ion battery, which is different from example 1 in that the thickness of the first material layer 1 is 3 μm, and the remaining parameters and experimental conditions are the same as those of example 1.
Example 7
The present example provides a method for preparing a positive electrode sheet of a lithium ion battery, which is different from example 1 in that the thickness of the first material layer 1 is 35 μm, and the remaining parameters and experimental conditions are the same as those of example 1.
Example 8
The present example provided a method for preparing a positive electrode sheet of a lithium ion battery, which is different from example 1 in that the thickness of the second material layer 2 is 15 μm, and the remaining parameters and experimental conditions are the same as those of example 1.
Example 9
The present example provided a method for preparing a positive electrode sheet of a lithium ion battery, which is different from example 1 in that the thickness of the second material layer 2 is 65 μm, and the remaining parameters and experimental conditions are the same as those of example 1.
Comparative example 1
The comparative example provides a method for preparing a positive plate of a lithium ion battery, wherein:
(1) Lithium supplementing material, positive electrode material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) In the mass ratio of 1:99, preparing the mixed active material powder by high-speed stirring and mixing;
(2) Conductive carbon black, conductive carbon tube, nitrogen methyl pyrrolidone solvent and polyvinylidene fluoride in a mass ratio of 1:0.5:40:1, dispersing and stirring for 2 hours at a high speed to prepare conductive slurry;
(3) Mixing the mixed active material powder with conductive slurry at a high speed, preparing positive electrode slurry with certain viscosity, uniformly coating the prepared slurry on an aluminum foil 33 by using a scraper to obtain a pole piece body, placing the pole piece body in a blast drying oven, drying for 20min at 120 ℃, rolling and cutting the dried pole piece under the pressure of 20MPa to prepare a positive electrode piece, and calculating the mass of the coating in unit volume at the moment, namely the compacted density of the pole piece.
Comparative example 2
The comparative example provides a method for preparing a positive plate of a lithium ion battery, which is different from example 1 in that the surface of the pole piece body is only coated with a first material layer 1, and the rest parameters and experimental conditions are the same as those of example 1.
Comparative example 3
The comparative example provides a method for preparing a positive plate of a lithium ion battery, which is different from the embodiment 1 in that the mass ratio of the lithium ion supplementary material to the positive material in the second material layer 2 coated on the surface of the pole piece body is greater than the mass ratio of the lithium ion supplementary material to the positive material in the first material layer 1, and the rest parameters and experimental conditions are the same as those of the embodiment 1.
The positive electrode sheets prepared in the examples and the comparative examples are respectively assembled into a 1Ah soft package battery for performance test, the test results are shown in Table 1, and the specific test steps are as follows:
after the formation and aging processes, the initial volume V of the 1Ah soft package battery prepared by using the drainage method is tested 0 The actual capacity of the battery is defined after one charge and discharge (the current density is 0.33C and the voltage window is 2.8-4.2V), the charge state of the battery is adjusted to 70% SOC, the battery is discharged for 30s at the current density of 4C, and the voltage difference value before and after the discharge is divided by the current density to be the direct current resistance value (DCR) of the battery under the charge State (SOC), so that the DCR values of 50% SOC and 20% SOC can be measured by the method.
And storing the battery in a constant temperature oven at 60 ℃, taking the battery out of the oven every 7 days, standing to room temperature, testing the volume of the battery, and charging the battery to 4.2V voltage at 0.33C current, wherein the volume change of the battery corresponds to the gas production of the battery core.
TABLE 1
As can be seen from the data in table 1:
as is evident from a comparison of example 1 and comparative example 1, the compaction, DCR, and gas storage properties of the cells coated with the first and second material layers 1 and 2 are superior to those of the cells without layered coating, because on the one hand the direct contact of the lithium supplementing material with the electrolyte is reduced, and the gas generation during the subsequent processes of the cells is reduced; on the other hand, the contact surface between the whole dressing layer and the foil is optimized, the direct current resistance of the battery is reduced, the internal resistance of the battery is comprehensively improved, and the stability of the battery is improved.
As can be seen from a comparison of example 1 and comparative example 2, the compaction, DCR, and stored gas production properties of the cells coated with the first material layer 1 are superior to those of the cells not coated with the first material layer 1, because on the one hand the direct contact of the lithium supplementing material with the electrolyte is reduced, and the gas production in the subsequent processes of the cells is reduced; on the other hand, the contact surface between the whole dressing layer and the foil is optimized, the direct current resistance of the battery is reduced, the internal resistance of the battery is comprehensively improved, and the stability of the battery is improved.
As is apparent from the comparison between example 1 and comparative example 3, the battery in which the mass ratio of the lithium ion supplement material and the cathode material in the second material layer 2 coated on the surface of the electrode sheet body in comparative example 3 is greater than that in the first material layer 1 has inferior compaction, DCR, and gas storage properties to the battery in example 1, because the content of the lithium supplement additive in the second material layer in comparative example 3 is high and the reaction with the electrolyte is severe, so that the compaction, DCR, and gas storage properties are deteriorated.
As is apparent from comparison of examples 1, 6 and 7, the present invention particularly defines that the thickness of the first material layer 1 is 5 to 30 μm, and if the thickness exceeds the limit value of 30 μm, it causes an increase in direct current internal resistance (DCR) due to the thickening of the dressing layer, which makes diffusion of lithium ions difficult; if the thickness thereof is less than the limit value of 5 μm, it may cause a decrease in the energy density of the battery due to insufficient lithium supplementing material.
As is apparent from comparison of examples 1, 8 and 9, the present invention particularly defines that the thickness of the second material layer 2 is 20 to 60 μm, and if the thickness exceeds the limit value of 60 μm, the direct current internal resistance (DCR) increases because the dressing layer becomes thick, and lithium ions are difficult to diffuse; if the thickness is less than the limit value of 20 μm, the stored gas yield increases because the first material layer is easily exposed to the electrolyte and side reactions continue to occur.
The applicant declares that the above is only a specific embodiment of the present invention, but the scope of the present invention is not limited thereto, and it should be apparent to those skilled in the art that any changes or substitutions that are easily conceivable within the technical scope of the present invention disclosed by the present invention fall within the scope of the present invention and the disclosure.
Claims (13)
1. The positive plate of the lithium ion battery is characterized by comprising a pole plate body, wherein a dressing layer is arranged on the surface of the pole plate body, the dressing layer comprises a first material layer and a second material layer which are sequentially laminated along the surface of the pole plate body, the first material layer comprises a lithium ion supplementing material and a positive electrode material, and the second material layer comprises a lithium ion supplementing material and a positive electrode material;
the mass ratio of the lithium ion supplementing material to the positive electrode material in the first material layer is larger than that of the lithium ion supplementing material to the positive electrode material in the second material layer;
the thickness of the first material layer is 5-30 mu m, and the thickness of the second material layer is 20-60 mu m;
the mass ratio of the lithium ion supplementary material to the positive electrode material in the first material layer is (1-5): (90-99), wherein the mass ratio of the lithium ion supplementary material to the positive electrode material in the second material layer is (0.1-1): (90-99).
2. The positive electrode sheet of claim 1, wherein the first material layer comprises a lithium ion supplemental material, a positive electrode material, conductive carbon black, conductive carbon tubes, and polyvinylidene fluoride.
3. The positive plate according to claim 2, wherein the mass ratio of the lithium ion supplementary material, the positive electrode material, the conductive carbon black, the conductive carbon tube and the polyvinylidene fluoride in the first material layer is (1-5): (90-99): 1:0.5:1.
4. the positive electrode sheet according to claim 1 or 2, wherein the second material layer comprises a lithium ion supplemental material, a positive electrode material, conductive carbon black, conductive carbon tube, and polyvinylidene fluoride.
5. The positive plate of claim 4, wherein the mass ratio of the lithium ion supplementary material, the positive electrode material, the conductive carbon black, the conductive carbon tube and the polyvinylidene fluoride in the second material layer is (0.1-1): (90-99): 1:0.5:1.
6. the positive electrode sheet according to claim 1, wherein the positive electrode material is lithium nickel cobalt manganate or lithium iron phosphate.
7. The positive electrode sheet according to claim 6, wherein the lithium nickel cobalt manganese oxide has a chemical formula of LiNi x Co y Mn 1-x-y O 2 Wherein x is more than or equal to 0.5 and less than or equal to 0.9, and y is more than or equal to 0 and less than or equal to 0.2.
8. The positive electrode sheet according to claim 6, wherein the lithium nickel cobalt manganese oxide is in a secondary spherical form or a single crystal form.
9. The positive electrode sheet according to claim 8, wherein the particle size of the secondary sphere of lithium nickel cobalt manganese oxide is 9-25 μm.
10. The positive electrode sheet according to claim 8, wherein the particle size of the nickel cobalt lithium manganate single crystal is 2 to 6 μm.
11. The positive electrode sheet according to claim 6, wherein the lithium iron phosphate is spherical lithium iron phosphate or nano lithium iron phosphate, the particle size of the spherical lithium iron phosphate is 6-15 μm, and the particle size of the nano lithium iron phosphate is 0.3-2.0 μm.
12. A method of producing the positive electrode sheet according to any one of claims 1 to 11, characterized in that the method comprises:
and sequentially laminating and coating a first material layer and a second material layer on the surface of the electrode plate body to form the positive electrode plate.
13. A lithium ion battery, characterized in that the lithium ion battery comprises a positive plate, a diaphragm and a negative plate which are sequentially laminated, wherein the positive plate adopts the positive plate according to any one of claims 1-11.
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