CN115172654B - Lithium supplementing negative electrode plate and secondary battery - Google Patents
Lithium supplementing negative electrode plate and secondary battery Download PDFInfo
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- CN115172654B CN115172654B CN202210875323.XA CN202210875323A CN115172654B CN 115172654 B CN115172654 B CN 115172654B CN 202210875323 A CN202210875323 A CN 202210875323A CN 115172654 B CN115172654 B CN 115172654B
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- lithium
- supplementing
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 61
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 60
- 230000001502 supplementing effect Effects 0.000 title claims abstract description 32
- 239000011248 coating agent Substances 0.000 claims abstract description 31
- 238000000576 coating method Methods 0.000 claims abstract description 31
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims abstract description 28
- 239000002245 particle Substances 0.000 claims abstract description 19
- 239000007773 negative electrode material Substances 0.000 claims abstract description 18
- 239000000463 material Substances 0.000 claims abstract description 16
- 230000001186 cumulative effect Effects 0.000 claims description 4
- 239000003792 electrolyte Substances 0.000 abstract description 22
- 229910001416 lithium ion Inorganic materials 0.000 abstract description 17
- 238000006243 chemical reaction Methods 0.000 abstract description 10
- 239000011149 active material Substances 0.000 abstract description 9
- 239000006183 anode active material Substances 0.000 abstract description 7
- 238000009792 diffusion process Methods 0.000 abstract description 6
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- 238000001035 drying Methods 0.000 description 12
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- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 8
- 239000011230 binding agent Substances 0.000 description 8
- 239000003960 organic solvent Substances 0.000 description 8
- 239000007774 positive electrode material Substances 0.000 description 8
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- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 7
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- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 6
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
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- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 2
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- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 229910015015 LiAsF 6 Inorganic materials 0.000 description 1
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 1
- 229910011281 LiCoPO 4 Inorganic materials 0.000 description 1
- 229910010707 LiFePO 4 Inorganic materials 0.000 description 1
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 description 1
- 229910002099 LiNi0.5Mn1.5O4 Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
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- 229910001128 Sn alloy Inorganic materials 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- QSNQXZYQEIKDPU-UHFFFAOYSA-N [Li].[Fe] Chemical compound [Li].[Fe] QSNQXZYQEIKDPU-UHFFFAOYSA-N 0.000 description 1
- OBNDGIHQAIXEAO-UHFFFAOYSA-N [O].[Si] Chemical compound [O].[Si] OBNDGIHQAIXEAO-UHFFFAOYSA-N 0.000 description 1
- BVDKLOSQZNHXSI-UHFFFAOYSA-N [Si].[Ni].[C] Chemical compound [Si].[Ni].[C] BVDKLOSQZNHXSI-UHFFFAOYSA-N 0.000 description 1
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- 229910045601 alloy Inorganic materials 0.000 description 1
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
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- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- 230000000977 initiatory effect Effects 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 239000002346 layers by function Substances 0.000 description 1
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 1
- 229910002102 lithium manganese oxide Inorganic materials 0.000 description 1
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 description 1
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000012466 permeate Substances 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
- 239000002985 plastic film Substances 0.000 description 1
- 229920006255 plastic film Polymers 0.000 description 1
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- 229910052718 tin Inorganic materials 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
- 229910001887 tin oxide Inorganic materials 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 229910052721 tungsten Inorganic materials 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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
-
- 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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M2010/4292—Aspects relating to capacity ratio of electrodes/electrolyte or anode/cathode
-
- 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 belongs to the technical field of secondary batteries, and particularly relates to a lithium supplementing negative electrode plate and a secondary battery, which comprise a negative electrode current collector and a negative electrode active coating arranged on at least one surface of the negative electrode current collector, wherein the negative electrode active coating comprises a negative electrode active material and a lithium supplementing material, and the lithium supplementing negative electrode plate meets the following relational expression: less than or equal to 0.13 [ [ (1000. Times. C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]and/(2.4-P) is less than or equal to 5.45. According to the invention, through reasonably matching the particle size, specific surface area and porosity of the anode active material and the surface density of the supplementary lithium element, the four materials meet a specific relation, a smooth lithium ion diffusion channel and a lithium ion reaction interface are constructed, the anode sheet is ensured to be infiltrated with proper lithium after being infiltrated by electrolyte, the lithium can rapidly infiltrate to the surface of the active material, the reaction is carried out on the surface of the anode sheet to form an SEI film, and the rest lithium ensures the cycle performance of the battery.
Description
Technical Field
The invention belongs to the technical field of secondary batteries, and particularly relates to a lithium supplementing negative electrode plate and a secondary battery.
Background
After the lithium supplementing technology is applied to the negative pole piece, the diaphragm and the positive pole piece are manufactured into a winding core in a winding/lamination mode, and electrolyte is injected after the winding core is assembled into a shell; at this time, lithium supplemented in the anode material passes through the electrolyte, namely, electrochemical reaction can occur spontaneously, and lithium ions form an SEI film on the surface of the anode material. The first lithium ion intercalation reaction, the intercalation depth of lithium ions, and the compactness degree of the surface SEI film can directly influence the first efficiency of the battery and DCR; the additional lithium can ensure the battery to have long cycle life; the current research work rarely limits the matching relation of the anode active material, the design of the anode piece and the lithium supplementing amount, and the anode material can not form a stable and firm interface when lithium ions are embedded for the first time, and correspondingly, the cycle life and the service life performance of the battery cannot be guaranteed.
Disclosure of Invention
One of the objects of the present invention is: aiming at the defects of the prior art, the lithium-supplementing negative electrode plate is provided, has stable and firm interface, and has longer cycle performance and service life.
In order to achieve the above purpose, the present invention adopts the following technical scheme:
the lithium supplementing negative electrode plate comprises a negative electrode current collector and a negative electrode active coating arranged on at least one surface of the negative electrode current collector, wherein the negative electrode active coating comprises a negative electrode active material and a lithium supplementing material, and the lithium supplementing negative electrode plate meets the following relational expression:
0.13≤[[(1000*C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]/(2.4-P)≤5.45；
wherein 1000 x C represents the area density of lithium element for supplementing lithium, and the unit is g/cm 2 ；
Wherein D50 represents the corresponding particle size in mu m when the cumulative particle size percentage of the negative electrode active material reaches 50%;
wherein P represents the porosity of the negative electrode piece in units;
wherein B represents the specific surface area of the negative electrode active material, and the unit is m 2 /g。
Preferably, the lithium-supplementing negative electrode sheet satisfies the following relation: less than or equal to 0.33 [ [ (1000. Times. C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]/(2.4-P)≤3.20；
Preferably, the 1000 XC has a value in the range of 0.02g/cm 2 ～1.57g/cm 2 。
Preferably, the 1000 XC has a value in the range of 0.10g/cm 2 ～1.08g/cm 2 。
Preferably, the D50 has a value ranging from 4 μm to 25. Mu.m.
Preferably, the D50 has a value ranging from 5 μm to 20. Mu.m.
Preferably, the value range of P is 20% -60%.
Preferably, the value range of P is 25% -45%.
Preferably, the value of B is 1.0cm 2 /g～6cm 2 /g。
Preferably, the value of B is 1.0cm 2 /g～4cm 2 /g。
The second object of the present invention is: aiming at the defects of the prior art, the secondary battery has the characteristics of high energy density and long service life.
In order to achieve the above purpose, the present invention adopts the following technical scheme:
a secondary battery comprises the lithium supplementing negative electrode plate.
Compared with the prior art, the invention has the beneficial effects that: according to the invention, through reasonably matching the particle size, specific surface area and porosity of the anode active material and the surface density of the supplementary lithium element, the four materials meet a specific relation, a smooth lithium ion diffusion channel and a lithium ion reaction interface are constructed, the anode sheet is ensured to be infiltrated with proper lithium after being infiltrated by electrolyte, the lithium can rapidly infiltrate to the surface of the active material, the reaction is carried out on the surface of the anode sheet to form an SEI film, and the rest lithium ensures the cycle performance of the battery.
Drawings
Fig. 1 is a schematic structural diagram of a lithium-compensating negative electrode sheet according to the present invention.
Fig. 2 is a second schematic structural diagram of the lithium-compensating negative electrode sheet of the present invention.
Fig. 3 is a third schematic structural view of the lithium-compensating negative electrode sheet of the present invention.
Wherein: 1. a negative electrode current collector; 2. a negative electrode active coating; 3. and (3) a lithium supplementing material.
Detailed Description
The invention will be described in further detail with reference to the following detailed description and the accompanying drawings, but the embodiments of the invention are not limited thereto.
The lithium supplementing negative electrode plate comprises a negative electrode current collector 1 and a negative electrode active coating 2 arranged on at least one surface of the negative electrode current collector 1, wherein the negative electrode active coating 2 comprises a negative electrode active material and a lithium supplementing material 3, and the lithium supplementing negative electrode plate meets the following relation:
0.13≤[[(1000*C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]/(2.4-P)≤5.45；
wherein 1000×C represents lithium element for supplementing lithiumSurface density in g/cm 2 ；
Wherein D50 represents the corresponding particle size in mu m when the cumulative particle size percentage of the negative electrode active material reaches 50%;
wherein P represents the porosity of the negative electrode piece in units;
wherein B represents the specific surface area of the negative electrode active material, and the unit is m 2 /g。
After the negative electrode piece for supplementing lithium is injected into the electrolyte, spontaneous electrochemical reaction of lithium and graphite occurs, and a compact and complete SEI film is formed. In order to ensure the compactness and completeness of the SEI film, the particle size, the specific surface area, the porosity of the negative electrode film and the surface density of the supplementary lithium element of the negative electrode active material are reasonably matched, so that the four materials meet a specific relation, a smooth lithium ion diffusion channel and a lithium ion reaction interface are constructed, the negative electrode film is ensured to be infiltrated by electrolyte, proper lithium can rapidly permeate to the surface of the active material and react on the surface of the active material to form the SEI film, and the residual lithium ensures the cycle performance of the battery.
The lithium-supplementing material 3 may be mixed with the raw materials in the negative electrode active coating 2 to form a mixed coating, as shown in fig. 3, and the lithium-supplementing material 3 may be formed into a lithium-supplementing layer alone, and may be disposed between the current collector and the negative electrode active coating 2, as shown in fig. 1, or may be disposed on a side of the negative electrode active coating 2 away from the current collector, as shown in fig. 2.
Wherein the particle size and specific surface area of the active material correspond to the interface at which lithium reacts with graphite: the particle size of the anode active material is small, lithium ions can be transmitted in particles, the diffusion speed and diffusion depth of the lithium ions in the anode active material are accelerated, but the specific surface area corresponding to the small particle size is large, more active lithium is consumed to form an SEI film, the SEI film occupation ratio is increased, and the interface impedance of a battery is increased; correspondingly, when the particle size of the anode active material is large, the diffusion depth of lithium ions is affected, but the specific surface area is correspondingly small, and consumed active lithium ions are reduced; particle size and specific surface area are 2 factors which are mutually influenced, and the balance of the particle size and the specific surface area is required to be sought to obtain better battery performance;
porosity of the negative electrode sheet: after the electrolyte is injected, electrochemical reaction of lithium ions and the anode material occurs, and the reaction speed and the reaction depth are related to the porosity of the anode piece; the porosity of the cathode is too high, the distance between the active material particles and the conductive agent is increased, the conductive network of the pole piece is poor, and the impedance of the battery is large; when the porosity of the cathode is too low, the previous contact of active substances is tight, but the electrochemical interface reaction is reduced, the charge transfer resistance is increased, the gap is too low, the permeation difficulty of electrolyte is increased, the active substances in the inner layer of the cathode pole piece are difficult to contact the electrolyte, the reaction state of the surface layer and the inner layer of the pole piece is uneven, and the long-term cycle performance of the battery is affected;
lithium element areal density of lithium supplement: when the lithium concentration in unit area is too high, the cathode is required to have more points for storing lithium elements, so that the energy density of the battery is limited; when the lithium concentration per unit area is insufficient, the reaction with the negative electrode active material is insufficient, which causes a difference in the shape of the local active material and also affects the long-term cycle performance.
Preferably, the lithium-supplementing negative electrode sheet satisfies the following relation: less than or equal to 0.33 [ [ (1000. Times. C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]/(2.4-P)≤3.20；
Preferably, the 1000 XC has a value in the range of 0.02g/cm 2 ～1.57g/cm 2 . The value of 1000 is 0.02g/cm 2 、0.04g/cm 2 、0.06g/cm 2 、0.08g/cm 2 、0.1g/cm 2 、0.108g/cm 2 、0.15g/cm 2 、0.20g/cm 2 、0.25g/cm 2 、0.30g/cm 2 、0.35g/cm 2 、0.4g/cm 2 、0.45g/cm 2 、0.8g/cm 2 、0.9g/cm 2 、1.1g/cm 2 、1.3g/cm 2 、1.5g/cm 2 、1.57g/cm 2 。
Preferably, the 1000 XC has a value in the range of 0.10g/cm 2 ～1.08g/cm 2 。
Preferably, the D50 has a value ranging from 4 μm to 25. Mu.m. The D50 values are 4 μm, 6 μm, 10 μm, 12 μm, 15 μm, 18 μm, 22 μm, 25 μm.
Preferably, the D50 has a value ranging from 5 μm to 20. Mu.m.
Preferably, the value range of P is 20% -60%. The value of P is 20%, 25%, 28%, 32%, 35%, 38%, 40%, 45%, 48%, 50%, 53%, 55%, 58%, 60%.
Preferably, the value range of P is 25% -45%.
Preferably, the value of B is 1.0cm 2 /g～6cm 2 And/g. The value of B is 1.0cm 2 /g、1.5cm 2 /g、1.8cm 2 /g、2.0cm 2 /g、2.2cm 2 /g、2.8cm 2 /g、3cm 2 /g、3.5cm 2 /g、3.9cm 2 /g、4.2cm 2 /g、4.7cm 2 /g、5.0cm 2 /g、5.5cm 2 /g、6cm 2 /g。
Preferably, the value of B is 1.0cm 2 /g～4cm 2 /g。
The second object of the present invention is: aiming at the defects of the prior art, the secondary battery has the characteristics of high energy density and long service life.
In order to achieve the above purpose, the present invention adopts the following technical scheme:
a secondary battery comprises the lithium supplementing negative electrode plate.
The positive electrode plate comprises a positive electrode active material, a conductive agent, a binder and a positive electrode current collector; the above 4 substances are not particularly limited and can be selected according to actual requirements; the positive electrode active material can be selected from lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, lithium nickel cobalt aluminum oxide, olivine-structured lithium-containing phosphate and the like; wherein the active material layer coated on the current collector of the positive electrode sheet can be a material of the formula such as Li a Ni x Co y M z O 2- b N b (wherein 0.95.ltoreq.a.ltoreq.1.2, x)>0, y is greater than or equal to 0, z is greater than or equal to 0, x+y+z=1, 0 is greater than or equal to b is greater than or equal to 1, M is selected from the combination of one or more of Mn and Al, N is selected from the combination of one or more of F, P and S), and the positive electrode active materialMay also be a material including but not limited to LiCoO 2 、LiNiO 2 、LiVO 2 、LiCrO 2 、LiMn 2 O 4 、LiCoMnO 4 、Li 2 NiMn 3 O 8 、LiNi 0.5 Mn 1.5 O 4 、LiCoPO 4 、LiMnPO 4 、LiFePO 4 、LiNiPO 4 、LiCoFSO 4 、CuS 2 、FeS 2 、MoS 2 、NiS、TiS 2 And the like. The positive electrode active material may be further subjected to a modification treatment, and a method for modifying the positive electrode active material should be known to those skilled in the art, for example, the positive electrode active material may be modified by coating, doping, or the like, and the material used for the modification treatment may be one or more combinations including, but not limited to, al, B, P, zr, si, ti, ge, sn, mg, ce, W, or the like. The positive current collector is usually a structure or a part for collecting current, and the positive current collector may be various materials suitable for being used as a positive current collector of a lithium ion battery in the field, for example, the positive current collector may be a metal foil, and the like, and more particularly may include, but is not limited to, an aluminum foil, and the like. The conductive agent can be selected from conductive carbon black, conductive graphite, VGCF, conductive carbon nano tube and graphene; the positive current collector can be aluminum foil, carbon-coated aluminum foil, porous aluminum foil, composite current collector, etc.
The negative electrode plate comprises a negative electrode active material, a conductive agent, a binder, a current collector and a lithium-containing layer; the above 5 substances are not particularly limited and can be selected according to actual requirements; for example, the negative electrode active material can be graphite, soft carbon, hard carbon, mesophase carbon microspheres, silicon-based materials, etc.; wherein the lithium-containing layer may be selected from: lithium powder, lithium belt, stabilized lithium metal powder lithium supplement, evaporation lithium supplement, electrochemical lithium supplement and the like; the active material layer coated on the current collector of the negative electrode sheet may be one or more of graphite, soft carbon, hard carbon, carbon fiber, mesophase carbon microsphere, silicon-based material, tin-based material, lithium titanate or other metals capable of forming an alloy with lithium, etc. Wherein, the graphite can be selected from one or more of artificial graphite, natural graphite and modified graphite; the silicon-based material can be one or more selected from simple substance silicon, silicon oxygen compound, silicon carbon compound and silicon alloy; the tin-based material can be selected from one or more of elemental tin, tin oxide and tin alloy. The negative electrode current collector 1 is generally a structure or a part for collecting current, and the negative electrode current collector 1 may be various materials suitable for use as a negative electrode current collector 1 of a lithium ion battery in the art, for example, the negative electrode current collector 1 may include, but is not limited to, a metal foil, etc., and more specifically may include, but is not limited to, a copper foil, etc.
The type of the diaphragm is not particularly limited, and can be selected according to actual requirements; for example, the membrane can be selected from polyethylene membrane, polypropylene membrane, polyvinylidene fluoride, non-woven fabric, etc.; meanwhile, the diaphragm can also be provided with different functional layers, such as an alumina coating, a boehmite coating, a PVDF coating and the like;
the lithium ion battery also includes an electrolyte comprising an organic solvent, an electrolyte lithium salt, and an additive. Wherein the electrolyte lithium salt can be LiPF used in high-temperature electrolyte 6 And/or LiBOB; liBF used in the low-temperature electrolyte may be used 4 、LiBOB、LiPF 6 At least one of (a) and (b); liBF used in the overcharge-preventing electrolyte may also be used 4 、LiBOB、LiPF 6 At least one of LiTFSI; liClO may also be 4 、LiAsF 6 、LiCF 3 SO 3 、LiN(CF 3 SO 2 ) 2 At least one of them. And the organic solvent may be a cyclic carbonate, including PC, EC; chain carbonates, including DFC, DMC, or EMC; carboxylic esters, including MF, MA, EA, MP, and the like, are also contemplated. And additives include, but are not limited to, film forming additives, conductive additives, flame retardant additives, overcharge prevention additives, and control of H in electrolytes 2 At least one of an additive for O and HF content, an additive for improving low temperature performance, and a multifunctional additive.
The shell, the shell material and shape are not particularly limited; for example, the shell can be a steel shell, an aluminum plastic film or the like.
Comparative example 1: a soft pack battery is exemplified;
1) Preparing a negative electrode plate:
mixing the negative electrode active material graphite, the conductive agent SP, the dispersing agent CMC and the binder LA133 according to the mass percentage of 96.7 percent to 1.0 percent to 0.8 percent to 1.5 percent, adding deionized water, and stirring the mixture into uniformly mixed stable slurry by a refiner; uniformly coating the obtained slurry on a current collector copper foil, drying, and cold pressing for later use;
2) Preparing a positive electrode plate:
mixing positive active material lithium iron phosphate, a conductive agent SP and a binder PVDF according to a certain mass ratio, adding NMP, and stirring by a refiner to obtain uniformly mixed stable slurry; uniformly coating the obtained slurry on a current collector aluminum foil, drying, and cold pressing for later use;
3) Preparing an electrolyte:
mixing Ethylene Carbonate (EC), ethylmethyl carbonate (EMC) and diethyl carbonate (DEC) according to a volume ratio of 1:1:1 to obtain an organic solvent, and then fully drying lithium salt LiPF 6 Dissolving in a mixed organic solvent to prepare electrolyte with the concentration of 1.0 mol/L;
4) Preparation of a diaphragm: selecting 9 mu m polyethylene film, coating Al on one side surface 2 O 3 A coating;
5) Preparation of electrode assemblies
Winding the positive electrode plate, the diaphragm and the negative electrode plate to enable the diaphragm to be positioned between the positive electrode plate and the negative electrode plate; and (3) placing the wound battery cell in a shell, drying, filling liquid, packaging, standing, and performing formation and activation to prepare the soft package battery with the battery cell capacity of 2.2 Ah.
Example 1: a soft pack battery is exemplified;
1) Preparing a negative electrode plate:
mixing negative electrode active material graphite, a conductive agent SP, a dispersing agent CMC, a binder LA133 and a lithium supplementing material 3 according to the mass percentage of 90.7 percent to 1.0 percent to 0.8 percent to 1.5 percent to 6 percent, adding deionized water, and stirring into uniformly mixed stable slurry by a refiner; uniformly coating the obtained slurry on a current collector copper foil, drying, and cold pressing for later use; the lithium supplementing negative electrode sheet meets the following relation:
0.13≤[[(1000*C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]/(2.4-P)≤5.45；
wherein 1000 x C represents the area density of lithium element for supplementing lithium, and the unit is g/cm 2 ；
Wherein D50 represents the corresponding particle size in mu m when the cumulative particle size percentage of the negative electrode active material reaches 50%;
wherein P represents the porosity of the negative electrode piece in units;
wherein B represents the specific surface area of the negative electrode active material, and the unit is m 2 /g。
2) Preparing a positive electrode plate:
mixing positive active material lithium iron phosphate, a conductive agent SP and a binder PVDF according to a certain mass ratio, adding NMP, and stirring by a refiner to obtain uniformly mixed stable slurry; uniformly coating the obtained slurry on a current collector aluminum foil, drying, and cold pressing for later use;
3) Preparing an electrolyte:
mixing Ethylene Carbonate (EC), ethylmethyl carbonate (EMC) and diethyl carbonate (DEC) according to a volume ratio of 1:1:1 to obtain an organic solvent, and then fully drying lithium salt LiPF 6 Dissolving in a mixed organic solvent to prepare electrolyte with the concentration of 1.0 mol/L;
4) Preparation of a diaphragm: selecting 9 mu m polyethylene film, coating Al on one side surface 2 O 3 A coating;
5) Preparation of electrode assemblies
Winding the positive electrode plate, the diaphragm and the negative electrode plate to enable the diaphragm to be positioned between the positive electrode plate and the negative electrode plate; and (3) placing the wound battery cell in a shell, drying, filling liquid, packaging, standing, and performing formation and activation to prepare the soft package battery with the battery cell capacity of 2.2 Ah.
The batteries prepared in comparative example 1 and examples 1 to 4 were subjected to 3000 charge and discharge tests according to example 1 and the different parameters set in the following tables, and the capacity retention was measured, and table 1 was recorded.
TABLE 1
Comparative example 1 is an uncompensated lithium group of a conventional lithium iron phosphate-graphite system, with a lithium element concentration per unit area of 1000×c=0 g/cm 2 At this time, the calculated value is a=0, and the range provided in this patent is not satisfied. The battery under the design has the advantages of no improvement of initial efficiency, larger DCR and limited cycle life. In the embodiment 1, a certain amount of lithium is given by calendaring and supplementing lithium, meanwhile, the selection of graphite materials and the design of pole pieces are limited, the energy density of the battery is high at the moment, but the initial effect is improved obviously, the DCR capacity retention rate is improved compared with the group without supplementing lithium, but the improvement effect is not obvious; example 2&3, the graphite materials are the same, the lithium supplementing amount is the same, the porosity of the negative electrode plate is different, the group with large porosity has slightly lower first effect from the actual result, but the DCR has greatly improved cycle capacity retention rate compared with the comparative example 1; in the embodiment 4, four design parameters are compounded, the calculated A value is 1.51, and the first effect, DCR and capacity retention rate are greatly improved; the above comparative examples are all obviously improved in performance under the condition of meeting the given range of the patent, only the difference of battery designs, and the improvement amplitude of three parameters of DCR and capacity retention rate is different for initial efficiency, so that the further targeted design can be specifically carried out according to the difference of the energy density requirements of the battery cells.
Comparative example 2: a soft pack battery is exemplified;
1) Preparing a negative electrode plate:
mixing a silicon-carbon anode active material, a conductive agent SP, a binder LA133 and a dispersing agent CMC according to the mass ratio of 97.0 percent to 0.6 percent to 1.0 percent to 1.4 percent, adding deionized water, and stirring by a refiner to form uniformly mixed stable slurry; uniformly coating the obtained slurry on a current collector copper foil, drying, and cold pressing for later use;
2) Preparing a positive electrode plate:
mixing positive electrode active material NCM811, conductive agent SP, conductive agent CNT and binder PVDF according to the mass ratio of 97.6 percent to 0.85 percent to 0.70 percent, adding NMP, and stirring into uniformly mixed stable slurry by a refiner; uniformly coating the obtained slurry on a current collector aluminum foil, drying, and cold pressing for later use;
3) Preparing an electrolyte:
mixing Ethylene Carbonate (EC), ethylmethyl carbonate (EMC) and diethyl carbonate (DEC) according to a volume ratio of 1:1:1 to obtain an organic solvent, and then fully drying lithium salt LiPF 6 Dissolving in a mixed organic solvent to prepare electrolyte with the concentration of 1.0 mol/L;
4) Preparation of a diaphragm: selecting 9 mu m polyethylene film, coating Al on one side surface 2 O 3 Coating, namely coating PVDF coating on two sides;
5) Preparation of electrode assemblies
Winding the positive electrode plate, the diaphragm and the negative electrode plate to enable the diaphragm to be positioned between the positive electrode plate and the negative electrode plate; and placing the wound battery core in a shell, drying, filling liquid, packaging, standing, and activating to prepare the soft package battery with the capacity of 3.1 Ah.
Examples 5 to 8 were set according to the different parameters of comparative example 2 and the following tables, and the batteries prepared in comparative example 2 and examples 5 to 8 were subjected to 3000 charge and discharge tests, test capacity retention rates, and record table 2.
TABLE 2
Comparative example 2 is an uncompensated lithium group of a high nickel-silicon carbon system, with a lithium element concentration per unit area of 1000×c=0 g/cm 2 At this time, the calculated value is a=0, and the range provided in this patent is not satisfied. The battery with the design has the advantages of no improvement of initial efficiency, larger DCR and limited cycle life; example 5&6, the cathode materials are the same, the lithium supplementing amounts are different, the porosity of the cathode pole piece is the same, and from the actual results, the group 8 with large lithium supplementing amount has greatly improved performances in all aspects compared with the comparative example 2 and the example 5; in the embodiment 7, four design parameters are compounded, the design is in a limit condition, and the first effect, DCR and capacity retention rate are greatly improved; example 8 Battery design was optimized accordinglyPorosity, performance is also equivalent; but example 7&8 are all other performance improvements obtained at the expense of energy density. Therefore, the selection of the parameters can be specifically designed in a further targeted manner according to the difference of the energy density requirements of the battery cells.
Variations and modifications of the above embodiments will occur to those skilled in the art to which the invention pertains from the foregoing disclosure and teachings. Therefore, the present invention is not limited to the above-described embodiments, but is intended to be capable of modification, substitution or variation in light thereof, which will be apparent to those skilled in the art in light of the present teachings. In addition, although specific terms are used in the present specification, these terms are for convenience of description only and do not limit the present invention in any way.
Claims (9)
1. The lithium supplementing negative electrode plate is characterized by comprising a negative electrode current collector and a negative electrode active coating arranged on at least one surface of the negative electrode current collector, wherein the negative electrode active coating comprises a negative electrode active material and a lithium supplementing material, and the lithium supplementing negative electrode plate meets the following relational expression:
0.13≤[[(1000*C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]/(2.4-P)≤5.45；
wherein 1000 x C represents the area density of lithium element for supplementing lithium, and the unit is g/cm 2 The value range of 1000 xC is 0.02g/cm 2 ～1.57g/cm 2 ；
Wherein D50 represents the corresponding particle size in mu m when the cumulative particle size percentage of the negative electrode active material reaches 50%;
wherein P represents the porosity of the negative electrode piece in units;
wherein B represents the specific surface area of the negative electrode active material, in cm 2 And/g, wherein the value range of the B is 1.0cm 2 /g～6cm 2 /g。
2. The lithium-compensating negative electrode tab of claim 1, wherein the lithium-compensating negative electrode tab satisfies the following relationship:
0.33≤[[(1000*C/5) 0.5 ]*[(D50) 0.5 ]*(2+0.25B)]/(2.4-P)≤3.20。
3. the lithium-compensating negative electrode of claim 2, wherein the 1000 x c range is 0.10g/cm 2 ～1.08g/cm 2 。
4. The lithium-compensating negative electrode tab of claim 1 or 2, wherein the D50 has a value in the range of 4 μm to 25 μm.
5. The lithium-compensating negative electrode tab of claim 4, wherein the D50 has a value in the range of 5 μm to 20 μm.
6. The lithium-compensating negative electrode tab of claim 1 or 2, wherein the P has a value in the range of 20% to 60%.
7. The lithium-compensating negative electrode tab of claim 6, wherein P has a value in the range of 25% to 45%.
8. The lithium-compensating negative electrode tab of claim 1, wherein the value of B is in the range of 1.0cm 2 /g～4cm 2 /g。
9. A secondary battery comprising the lithium-supplementing negative electrode tab of any one of claims 1-8.
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| CN114122368A (en) * | 2020-08-28 | 2022-03-01 | 比亚迪股份有限公司 | Lithium supplement material, manufacturing method thereof, negative pole piece and battery |
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| CN113871574A (en) * | 2021-09-24 | 2021-12-31 | 远景动力技术(江苏)有限公司 | Lithium ion battery negative plate and preparation method and application thereof |
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