WO2022218143A1 - 一种磷酸铁锂电池 - Google Patents
一种磷酸铁锂电池 Download PDFInfo
- Publication number
- WO2022218143A1 WO2022218143A1 PCT/CN2022/083551 CN2022083551W WO2022218143A1 WO 2022218143 A1 WO2022218143 A1 WO 2022218143A1 CN 2022083551 W CN2022083551 W CN 2022083551W WO 2022218143 A1 WO2022218143 A1 WO 2022218143A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- group
- cyclic
- iron phosphate
- lithium iron
- positive electrode
- Prior art date
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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 title claims abstract description 54
- 150000001875 compounds Chemical class 0.000 claims abstract description 54
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims abstract description 53
- 239000011255 nonaqueous electrolyte Substances 0.000 claims abstract description 43
- 239000003792 electrolyte Substances 0.000 claims abstract description 25
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 22
- 239000007774 positive electrode material Substances 0.000 claims abstract description 20
- 239000002904 solvent Substances 0.000 claims abstract description 12
- 150000003839 salts Chemical class 0.000 claims abstract description 10
- 238000005056 compaction Methods 0.000 claims abstract description 9
- 125000004122 cyclic group Chemical group 0.000 claims description 88
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 18
- 125000004430 oxygen atom Chemical group O* 0.000 claims description 15
- 150000005676 cyclic carbonates Chemical group 0.000 claims description 14
- 125000001174 sulfone group Chemical group 0.000 claims description 14
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical group OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 claims description 13
- 150000007942 carboxylates Chemical group 0.000 claims description 13
- 125000004018 acid anhydride group Chemical group 0.000 claims description 12
- QAOWNCQODCNURD-UHFFFAOYSA-L sulfate group Chemical group S(=O)(=O)([O-])[O-] QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 12
- 125000000743 hydrocarbylene group Chemical group 0.000 claims description 11
- 125000001273 sulfonato group Chemical group [O-]S(*)(=O)=O 0.000 claims description 11
- 125000003375 sulfoxide group Chemical group 0.000 claims description 11
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- 150000002367 halogens Chemical class 0.000 claims description 8
- 229910052799 carbon Inorganic materials 0.000 claims description 7
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 7
- 125000006274 (C1-C3)alkoxy group Chemical group 0.000 claims description 6
- 150000008282 halocarbons Chemical group 0.000 claims description 4
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- 125000002947 alkylene group Chemical group 0.000 claims description 3
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- -1 iron ion Chemical class 0.000 abstract description 39
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Images
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- H01M2300/0025—Organic electrolyte
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- 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
Definitions
- the invention belongs to the technical field of secondary batteries, and particularly relates to a lithium iron phosphate battery.
- lithium-ion batteries Because of the advantages of high operating voltage, long cycle life, high energy density, and no memory effect, lithium-ion batteries have been widely used in mobile communications, notebook computers and other fields since they were put into the market in 1991. In recent years, with the rapid development and popularization of new energy vehicles, consumers have higher and higher requirements for the energy density of lithium-ion batteries. Compared with ternary batteries, lithium iron phosphate batteries are more advantageous in terms of cycle life, safety and cost, but the energy density of lithium iron phosphate is still far from that of ternary materials. The energy density is mainly achieved by increasing the compaction density of the lithium iron phosphate cathode.
- the present invention provides a lithium iron phosphate battery.
- the present invention provides a lithium iron phosphate battery, comprising a positive electrode, a negative electrode and a non-aqueous electrolyte, the positive electrode comprises a positive electrode material layer, the compaction density of the positive electrode material layer is 2.3-2.8 g/cc, and the positive electrode material the layer includes a positive active material including LiFePO 4 ;
- the non-aqueous electrolyte includes a solvent, an electrolyte salt, vinylene carbonate and a compound represented by structural formula 1:
- A, B and C are each independently selected from the group consisting of cyclic carbonate group, cyclic sulfate group, cyclic sulfite group, cyclic sulfonate group, cyclic sulfone group, cyclic sulfoxide group, A cyclic carboxylate group or a cyclic acid anhydride group;
- D and E are each independently selected from a single bond, or a group containing a hydrocarbylene group, an ether bond, a sulfur-oxygen double bond or a carbon-oxygen double bond;
- the addition amount of the compound represented by the structural formula 1 is 0.01 to 5%.
- the added amount of the vinylene carbonate is 0.01-5%, and more preferably, the added amount of the vinylene carbonate is 0.1-5% 2%.
- the surface of the positive electrode is detected by X-ray photoelectron spectroscopy, and when the 1s peak of carbon is obtained at 284.5eV, the characteristic peak of S appears in the region of 162-174eV.
- the charge-discharge voltage range of the lithium iron phosphate battery is 2.0-3.8V.
- A, B, and C independently contain a cyclic carbonate group, a cyclic sulfate group, a cyclic sulfite group, a cyclic sulfonate group, a cyclic sulfone group, and a cyclic sulfoxide group.
- the number of cyclic carboxylate groups and cyclic acid anhydride groups is 1 to 5
- A, B, and C contain cyclic carbonate groups, cyclic sulfate groups, cyclic sulfite groups, and cyclic sulfonic acid groups.
- the total number of ester groups, cyclic sulfone groups, cyclic sulfoxide groups, cyclic carboxylic acid ester groups and cyclic acid anhydride groups is less than or equal to 10.
- a and C are independently selected from the groups shown in structural formula 2:
- n is selected from an integer from 0 to 4
- R 1 is selected from hydrogen, halogen, C1-C5 hydrocarbon group or halogenated hydrocarbon group
- R 2 , R 3 , R 4 , R 5 , R 6 , R 7 are independently selected from each other From C1-C3 alkylene group, C1-C3 alkoxy group, oxygen atom
- At least one of R 2 , R 3 and R 4 is selected from And at least one of R 2 , R 3 and R 4 is selected from oxygen atoms
- at least one of R 5 , R 6 and R 7 is selected from And at least one of R 5 , R 6 and R 7 is selected from And at least one of R 5 , R 6 and R 7 is selected from oxygen atoms.
- B is selected from the group shown in structural formula 3:
- m is selected from an integer of 1 to 4
- R 8 , R 9 and R 10 are each independently selected from C1-C3 hydrocarbylene, C1-C3 alkoxy, oxygen atom, At least one of R 8 , R 9 and R 10 is selected from And at least one of R 8 , R 9 and R 10 is selected from oxygen atoms.
- D and E are each independently selected from the groups shown in structural formula 4:
- z is selected from an integer from 0 to 4
- R 11 and R 13 are each independently selected from a single bond or a C1-C5 hydrocarbylene group
- R 12 is selected from a single bond
- D and E are each independently selected from single bonds or C1-C5 alkylene groups
- A, B, and C are each independently selected from substituted or unsubstituted cyclic carbonate groups, cyclic sulfate groups, cyclic sulfite group, cyclic sulfonate group, cyclic sulfone group, cyclic sulfoxide group, cyclic carboxylate group or cyclic acid anhydride group, when A, B or C is substituted, the substituent is selected from halogen , alkyl or haloalkyl.
- a and C are the same as each other, A and B are the same or different from each other, and D and E are the same as each other.
- the compound shown in the structural formula 1 is selected from one or more of the following compounds:
- vinylene carbonate and the compound represented by the structural formula 1 are added to the non-aqueous electrolyte, wherein the vinylene carbonate and the compound represented by the structural formula 1 participate in the interface between the positive electrode and the negative electrode surface Film formation, it is presumed that the decomposition product of vinylene carbonate and the decomposition product of the compound represented by structural formula 1 together constitute an organic-inorganic interfacial film, which can effectively improve the migration of lithium ions during high temperature cycling of the battery.
- Fig. 1 is the full spectrum of the XPS spectrum of the positive electrode sheet of the battery provided by the embodiment of the present invention after the battery is divided;
- Fig. 2 is the fine spectrum of characteristic peak in Fig. 1;
- Example 3 is a SEM image of the negative electrode after 1000 cycles of the battery provided in Example 5 of the present invention.
- FIG. 4 is a SEM image of the negative electrode of the battery provided in Comparative Example 1 of the present invention after 1000 cycles.
- An embodiment of the present invention provides a lithium iron phosphate battery, including a positive electrode, a negative electrode and a non-aqueous electrolyte, the positive electrode includes a positive electrode material layer, and the compaction density of the positive electrode material layer is 2.3-2.8 g/cc, and the The positive electrode material layer includes a positive electrode active material, and the positive electrode active material includes LiFePO 4 ;
- the non-aqueous electrolyte includes a solvent, an electrolyte salt, vinylene carbonate and a compound represented by structural formula 1:
- A, B and C are each independently selected from groups containing cyclic ester groups or cyclic acid anhydride groups, and the cyclic ester groups include cyclic carbonate groups, cyclic sulfate groups, cyclic sulfite groups One or more of cyclic sulfonate group, cyclic sulfonate group, cyclic sulfone group, cyclic sulfoxide group and cyclic carboxylate group;
- D and E are each independently selected from a single bond, or a group containing a hydrocarbylene group, an ether bond, a sulfur-oxygen double bond or a carbon-oxygen double bond;
- the addition amount of the compound represented by the structural formula 1 is 0.01 to 5%.
- the inventors speculated that vinylene carbonate and the compound represented by structural formula 1 participated in the formation of the interface film on the surface of the positive electrode and the negative electrode, and the decomposition product of vinylene carbonate and the compound represented by structural formula 1 jointly formed an organic compound.
- the interfacial film can effectively improve the migration rate of lithium ions during the high temperature cycle of the battery, and at the same time has a good protective effect on the electrode material, reducing the redox reaction between the electrolyte and the electrode material, The formation of lithium dendrites at the interface of the negative electrode and the dissolution of Fe ions from the positive electrode are inhibited, and the high temperature and safety performance of the lithium iron phosphate battery are finally improved.
- Vinylene carbonate can form an organic interface of polymer structure on the surface of the electrode, but in the high-density lithium iron phosphate system, this organic interface on the negative electrode is not conducive to the migration of lithium ions, which will deposit on the surface of the negative electrode Lithium dendrites are formed, and the reaction between lithium dendrites and electrolyte causes further deterioration of battery performance and iron ion dissolution.
- the inventor found through experiments that when vinylene carbonate and structural formula 1 are added to the non-aqueous electrolyte at the same time. When the compound of structural formula 1 is added, it can form a better coordination effect with the lithium iron phosphate battery of high compaction density.
- the compound of structural formula 1 When the compound of structural formula 1 is added, the compound of structural formula 1 can form an interface film containing special components on the electrode surface. That is, the lithium ion conduction rate of the interface film can be improved, the structure of the positive and negative electrodes can be protected, and the stability of the battery material under high temperature cycling can be improved.
- the addition amount of the compound represented by the structural formula 1 is 0.1-2%.
- the surface of the positive electrode is detected by X-ray photoelectron spectroscopy.
- the 1s peak of carbon is obtained at 284.5eV
- the characteristic peak of S appears in the region of 162-174eV, as shown in Figure 1 and Figure 2
- the interface film has relatively excellent organic and inorganic compositions, and the performance of high-pressure lithium iron phosphate batteries is significantly improved.
- the vinylene carbonate is added in an amount of 0.01-5% based on 100% of the total mass of the non-aqueous electrolyte.
- the addition amount of the vinylene carbonate is 0.1-2%.
- the vinylene carbonate and the compound represented by the structural formula 1 have a good coordination relationship, and when the addition amount of either vinylene carbonate or the compound represented by the structural formula 1 is too low, it is difficult to Produces a better blending effect; when the amount of vinylene carbonate or any of the compounds shown in structural formula 1 is too much, not only will the film be too thick, resulting in an increase in impedance, but also significantly increase the viscosity of the electrolyte, affecting the battery. performance.
- the charge-discharge voltage range of the lithium iron phosphate battery is 2.0-3.8V.
- A, B, and C each independently contain a cyclic carbonate group, a cyclic sulfate group, a cyclic sulfite group, a cyclic sulfonate group, a cyclic sulfone group, a cyclic sulfite group
- the number of sulfone group, cyclic carboxylate group and cyclic acid anhydride group is 1 to 5, and A, B, C cyclic carbonate group, cyclic sulfate group, cyclic sulfite group, cyclic sulfonic acid group
- the total number of ester groups, cyclic sulfone groups, cyclic sulfoxide groups, cyclic carboxylate groups and cyclic acid anhydride groups is less than or equal to 10.
- a and C are each independently selected from groups represented by structural formula 2:
- n is selected from an integer from 0 to 4
- R 1 is selected from hydrogen, halogen, C1-C5 hydrocarbon group or halogenated hydrocarbon group
- R 2 , R 3 , R 4 , R 5 , R 6 , R 7 are independently selected from each other From C1-C3 alkylene group, C1-C3 alkoxy group, oxygen atom
- At least one of R 2 , R 3 and R 4 is selected from And at least one of R 2 , R 3 and R 4 is selected from oxygen atoms
- at least one of R 5 , R 6 and R 7 is selected from And at least one of R 5 , R 6 and R 7 is selected from And at least one of R 5 , R 6 and R 7 is selected from oxygen atoms.
- the combined group of -R 3 -R 2 -R 4 - and the combined group of -R 7 -R 5 -R 6 - are each independently selected from
- B is selected from the group represented by Structural Formula 3:
- m is selected from an integer of 1 to 4
- R 8 , R 9 and R 10 are each independently selected from C1-C3 hydrocarbylene, C1-C3 alkoxy, oxygen atom, At least one of R 8 , R 9 and R 10 is selected from And at least one of R 8 , R 9 and R 10 is selected from oxygen atoms.
- the combined groups of -R 9 -R 8 -R 10 - are each independently selected from
- D and E are each independently selected from groups represented by structural formula 4:
- z is selected from an integer from 0 to 4
- R 11 and R 13 are each independently selected from a single bond or a C1-C5 hydrocarbylene group
- R 12 is selected from a single bond
- a and C are the same as each other, A and B are the same or different from each other, and D and E are the same as each other.
- the compound represented by the structural formula 1 is a symmetrical structure, and the compound represented by the structural formula 1 of the symmetrical structure is easier to synthesize than the asymmetrical structure, The yield of the product is higher, which is beneficial to reduce the production cost.
- D and E are each independently selected from single bonds or C1-C5 hydrocarbylene groups
- A, B, and C are each independently selected from substituted or unsubstituted cyclic carbonate groups, cyclic sulfate groups , cyclic sulfite group, cyclic sulfonate group, cyclic sulfone group, cyclic sulfoxide group, cyclic carboxylate group or cyclic acid anhydride group, preferably, when A, B or C is substituted,
- the substituent is selected from halogen, hydrocarbyl or halohydrocarbyl, more preferably, when A, B or C is substituted, the substituent is selected from halogen, alkyl or haloalkyl.
- the compound represented by structural formula 1 can be selected from one or more of the following compounds:
- D and E are each independently selected from groups represented by structural formula 4:
- z is selected from an integer of 1-4
- R 11 and R 13 are each independently selected from a single bond or a C1-C5 hydrocarbylene group
- R 12 is selected from
- A, B and C are each independently selected from substituted or unsubstituted cyclic carbonate groups, cyclic sulfate groups, cyclic sulfite groups, cyclic sulfonate groups, cyclic sulfone groups, cyclic sulfoxide groups group, cyclic carboxylate group or cyclic acid anhydride group, preferably, when A, B or C is substituted, the substituent is selected from halogen, hydrocarbon group or halogenated hydrocarbon group, more preferably, when A, B or C is substituted , the substituents are selected from halogen, alkyl or haloalkyl.
- the compound represented by structural formula 1 can be selected from one or more of the following compounds:
- the compound represented by the structural formula 1 can also be selected from one or more of the following compounds:
- Compound 1 can be prepared by the following methods:
- the organic solvents such as sorbitol, dimethyl carbonate, methanol alkaline substance catalyst potassium hydroxide and DMF are placed in the reaction vessel, and after reacting for several hours under heating conditions, a certain amount of oxalic acid is added to adjust the pH to neutrality, and the solution is filtered. After recrystallization, intermediate product 1 can be obtained, and then intermediate product 1, carbonate, thionyl chloride, etc. are esterified under high temperature conditions to obtain intermediate product 2, and then intermediate product 2 is obtained by using an oxidant such as sodium periodate. Compound 1 can be obtained by oxidation.
- Compound 2 can be made by:
- the solvent includes one or more of ether-based solvents, nitrile-based solvents, carbonate-based solvents, and carboxylate-based solvents.
- the ether solvent includes cyclic ether or chain ether.
- cyclic ethers examples include 1,3-dioxolane (DOL), 1,4-dioxoxane (DX), crown ethers, tetrahydrofuran (THF), 2-methyltetrahydrofuran (2 -CH3 -THF), one or more of 2-trifluoromethyltetrahydrofuran (2- CF3 -THF).
- DOL 1,3-dioxolane
- DX 1,4-dioxoxane
- crown ethers examples include tetrahydrofuran (THF), 2-methyltetrahydrofuran (2 -CH3 -THF), one or more of 2-trifluoromethyltetrahydrofuran (2- CF3 -THF).
- chain ethers examples include one or more of dimethoxymethane (DMM), 1,2-dimethoxyethane (DME), and diglyme (TEGDME) .
- DDM dimethoxymethane
- DME 1,2-dimethoxyethane
- TEGDME diglyme
- nitrile-based solvent one or more of acetonitrile, glutaronitrile, and malononitrile can be mentioned.
- carbonate-based solvents include cyclic carbonates or chain carbonates.
- cyclic carbonates include one or more of ethylene carbonate (EC), propylene carbonate (PC), ⁇ -butyrolactone (GBL), and butylene carbonate (BC).
- EC ethylene carbonate
- PC propylene carbonate
- GBL ⁇ -butyrolactone
- BC butylene carbonate
- chain carbonates examples include dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), diethyl carbonate (DEC), methyl-n-propyl carbonate, ethyl-n-propyl carbonate One or more of ester, dipropyl carbonate (DPC).
- DMC dimethyl carbonate
- EMC ethyl methyl carbonate
- DEC diethyl carbonate
- methyl-n-propyl carbonate ethyl-n-propyl carbonate
- DPC dipropyl carbonate
- the carboxylate solvent includes cyclic carboxylate or chain carbonate.
- cyclic carboxylic acid esters include one or more of ⁇ -butyrolactone, ⁇ -valerolactone, and ⁇ -valerolactone.
- chain carbonates examples include methyl acetate (MA), ethyl acetate (EA), propyl acetate (EP), butyl acetate, propyl propionate (PP), and butyl propionate. one or more of.
- the electrolyte salt is selected from lithium salts.
- the electrolyte salt is selected from LiPF 6 , LiBF 4 , LiBOB, LiDFOB, LiN(SO 2 CF 3 ) 2 , LiN(SO 2 C 2 F 5 ) 2 , LiC(SO 2 CF 3 ) 3 , LiN(SO 2 F) 2 , LiClO 4 , LiAsF 6 , LiSbF 6 , LiCF 3 SO 3 , Li 2 B 10 Cl 10 , lithium lower aliphatic carboxylate, LiAlCl 4 , LiDFOP, LiPO 2 F 2 one or more.
- the electrolyte salt is selected from one or more of LiPF 6 , LiPO 2 F 2 and LiFSI.
- the concentration of the electrolyte salt in the non-aqueous electrolyte, is 0.1 mol/L-8 mol/L. In a preferred embodiment, in the non-aqueous electrolyte, the concentration of the electrolyte salt is 0.5mol/L-4mol/L. Specifically, the concentration of the electrolyte salt may be 0.5 mol/L, 1 mol/L, 1.5 mol/L, 2 mol/L, 2.5 mol/L, 3 mol/L, 3.5 mol/L or 4 mol/L.
- the non-aqueous electrolyte further includes auxiliary additives
- the auxiliary additives include fluorinated cyclic carbonate compounds, sultone compounds, aromatic additives, fluorinated anisole compounds, dicarboxylic acid Acid Anhydride, Lithium Difluorophosphate, Vinyl Sulfate (DTD), Lithium Bisfluorosulfonimide (LiFSI), Methylene Methylene Disulfonate, Tris(trimethylsilane) Phosphate, Tris(trimethylsilane) ) at least one of borate esters.
- the fluorinated cyclic carbonate compounds include fluoroethylene carbonate (FEC), 4,4-difluoroethylene carbonate, 4,5-difluoroethylene carbonate, 4- Fluoro-4-methylethylene carbonate, 4,5-difluoro-4-methylethylene carbonate, 4-fluoro-5-methylethylene carbonate, 4,4-difluoro-5-methyl Ethylene carbonate, 4-(fluoromethyl) ethylene carbonate, 4-(difluoromethyl) ethylene carbonate, 4-(trifluoromethyl) ethylene carbonate, 4-(fluoromethyl) )-4-fluoroethylene carbonate, 4-(fluoromethyl)-5-fluoroethylene carbonate, 4-fluoro-4,5-dimethylethylene carbonate, 4,5-difluoro-4 , one or more of 5-dimethyl ethylene carbonate and 4,4-difluoro-5,5-dimethyl ethylene carbonate.
- FEC fluoroethylene carbonate
- the non-aqueous electrolyte contains fluorinated cyclic carbonate compounds, based on the total mass of the non-aqueous electrolyte as 100%, the content of the fluorinated cyclic carbonate compounds is 0.1-30% ;
- the sultone compound is selected from 1,3-propane sultone (PS), 1,4-butane sultone (BS), 1,3-propene sultone ( one or more of PST).
- the mass percentage of the sultone compounds is 0.1-5% .
- the aromatic additives include biphenyls, alkyl biphenyls, terphenyls, partial hydrides of terphenyls, cyclohexylbenzene, tert-butylbenzene, tert-amylbenzene, diphenyl ether, diphenyl Aromatic compounds such as furan; one or more of 2-fluorobiphenyl, o-cyclohexyl fluorobenzene and p-cyclohexyl fluorobenzene.
- the mass percentage content of the aromatic additives is 0.1-5% based on the total mass of the non-aqueous electrolyte as 100%.
- the fluoroanisole compound includes one or more of 2,4-difluoroanisole, 2,5-difluoroanisole, and 2,6-difluoroanisole.
- the mass percentage of the fluorine-containing anisole compound is 0.1-5%.
- the dicarboxylic anhydride includes one or more of succinic acid, maleic acid, and phthalic acid.
- the mass percentage of the dicarboxylic anhydride is 0.1-5% based on the total mass of the non-aqueous electrolyte as 100%.
- the mass percentage of the lithium difluorophosphate is 0.1- 2%;
- the non-aqueous electrolyte contains vinyl sulfate (DTD), based on the total mass of the non-aqueous electrolyte as 100%, the mass percentage of the vinyl sulfate (DTD) The content is 0.1-5%;
- the non-aqueous electrolyte contains lithium bis(fluorosulfonyl)imide (LiFSI), based on 100% of the total mass of the non-aqueous electrolyte, the bis(fluorosulfonyl) The mass percentage content of lithium imide (LiFSI) is 0.1-5%.
- the auxiliary additives further include 1-methyl-2-pyrrolidone, 1-methyl-2-piperidone, 3-methyl-2-oxazolidinone, 1,3-dimethylone Nitrogen-containing compounds such as base-2-imidazolidinone and N-methylsuccinimide; hydrocarbon compounds such as heptane, octane, and cycloheptane; fluorine-containing aromatic compounds such as fluorobenzene, difluorobenzene, and trifluorotoluene Wait.
- Nitrogen-containing compounds such as base-2-imidazolidinone and N-methylsuccinimide
- hydrocarbon compounds such as heptane, octane, and cycloheptane
- fluorine-containing aromatic compounds such as fluorobenzene, difluorobenzene, and trifluorotoluene Wait.
- the mass percentage content of any optional substance in the auxiliary additives in the non-aqueous electrolyte solution is in the range of 10% or less, preferably, the mass percentage content is 0.1% -5%.
- the auxiliary additive is selected from one or more of 1,3-propane sultone, methylene methanedisulfonate, fluoroethylene carbonate and vinyl sulfate.
- the positive electrode further includes a positive electrode current collector, and the positive electrode material layer covers the surface of the positive electrode current collector.
- the positive electrode current collector is selected from metal materials that can conduct electrons.
- the positive electrode current collector includes one or more of Al, Ni, and stainless steel.
- the positive electrode current collector is selected from the group consisting of: aluminum foil.
- the positive electrode material layer further includes a positive electrode binder and a positive electrode conductive agent, and the positive electrode active material, the positive electrode binder and the positive electrode conductive agent are blended to obtain the positive electrode material layer.
- the positive electrode binder includes polyvinylidene fluoride, vinylidene fluoride copolymer, polytetrafluoroethylene, vinylidene fluoride-hexafluoropropylene copolymer, tetrafluoroethylene-hexafluoropropylene copolymer, tetrafluoroethylene- Perfluoroalkyl vinyl ether copolymer, ethylene-tetrafluoroethylene copolymer, vinylidene fluoride-tetrafluoroethylene copolymer, vinylidene fluoride-trifluoroethylene copolymer, vinylidene fluoride-trichloroethylene copolymer Copolymers, vinylidene fluoride-vinyl fluoride copolymers, vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene copolymers, thermoplastic polyimides, thermoplastic resins such as polyethylene and polypropylene; acrylic resins;
- the positive electrode conductive agent includes one or more of conductive carbon black, conductive carbon balls, conductive graphite, conductive carbon fibers, carbon nanotubes, graphene or reduced graphene oxide.
- the negative electrode includes a negative electrode material layer, the negative electrode material layer includes a negative electrode active material, and the negative electrode active material includes one or more of a silicon-based negative electrode, a carbon-based negative electrode, a tin-based negative electrode, and a lithium negative electrode kind.
- the silicon-based negative electrode includes one or more of silicon material, silicon oxide, silicon-carbon composite material and silicon alloy material;
- the carbon-based negative electrode includes graphite, hard carbon, soft carbon, graphene, intermediate One or more of phase carbon microspheres;
- the tin-based negative electrode includes one or more of tin, tin carbon, tin oxygen, and tin metal compounds;
- the lithium negative electrode includes one or more of metallic lithium or lithium alloys. one or more.
- the lithium alloy may be at least one of a lithium-silicon alloy, a lithium-sodium alloy, a lithium-potassium alloy, a lithium-aluminum alloy, a lithium-tin alloy, and a lithium-indium alloy.
- the negative electrode active material is selected from one or more of artificial graphite, natural graphite and siloxane.
- the negative electrode further includes a negative electrode current collector, and the negative electrode material layer covers the surface of the negative electrode current collector.
- the negative electrode current collector is selected from metal materials that can conduct electrons.
- the negative electrode current collector includes one or more of Cu, Ni, and stainless steel.
- the negative electrode current collector is selected from the group consisting of: copper foil.
- the negative electrode material layer further includes a negative electrode binder and a negative electrode conductive agent, and the negative electrode material layer is obtained by blending the negative electrode active material, the negative electrode binder and the negative electrode conductive agent.
- the negative electrode binder includes polyvinylidene fluoride, vinylidene fluoride copolymer, polytetrafluoroethylene, vinylidene fluoride-hexafluoropropylene copolymer, tetrafluoroethylene-hexafluoropropylene copolymer, tetrafluoroethylene- Perfluoroalkyl vinyl ether copolymer, ethylene-tetrafluoroethylene copolymer, vinylidene fluoride-tetrafluoroethylene copolymer, vinylidene fluoride-trifluoroethylene copolymer, vinylidene fluoride-trichloroethylene copolymer Copolymers, vinylidene fluoride-vinyl fluoride copolymers, vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene copolymers, thermoplastic polyimides, thermoplastic resins such as polyethylene and polypropylene; acrylic resins;
- the negative electrode conductive agent includes one or more of conductive carbon black, conductive carbon ball, conductive graphite, conductive carbon fiber, carbon nanotube, graphene or reduced graphene oxide.
- the battery further includes a separator located between the positive electrode and the negative electrode.
- the separator can be an existing conventional separator, which can be a ceramic separator, a polymer separator, a non-woven fabric, an inorganic-organic composite separator, etc., including but not limited to single-layer PP (polypropylene), single-layer PE (polyethylene), Diaphragms such as double-layer PP/PE, double-layer PP/PP and triple-layer PP/PE/PP.
- the cathode active material lithium iron phosphate, conductive carbon black Super-P, and binder polyvinylidene fluoride (PVDF) were mixed in a mass ratio of 93:4:3, and then dispersed in N-methyl-2-pyrrolidone ( NMP), the positive electrode slurry was obtained.
- NMP N-methyl-2-pyrrolidone
- the slurry is evenly coated on both sides of the aluminum foil, dried, calendered and vacuum-dried, and the aluminum lead wire is welded with an ultrasonic welder to obtain a positive electrode plate.
- the thickness of the electrode plate is 120-150 ⁇ m.
- the true densities are shown in the following tables.
- a polyethylene microporous film with a thickness of 20 ⁇ m was placed between the positive plate and the negative plate as a separator, and then the sandwich structure composed of the positive plate, the negative plate and the separator was wound, and the rolled body was flattened and placed in aluminum plastic.
- the aluminum-plastic film is hot-pressed and sealed to obtain the battery core to be injected.
- the electrolyte prepared above is injected into the cell through the liquid injection hole, and the amount of electrolyte should ensure that the gap in the cell is filled. Then it is formed according to the following steps: 0.05C constant current charging for 180min, 0.1C constant current charging for 180min, rest for 24hrs, shape and seal, and then further charge to 3.65V with 0.2C current and constant current, after 24hrs at room temperature, charge at 0.2C Current constant current discharge to 2.0V.
- Capacity retention rate (1000th discharge capacity ⁇ 1st week discharge capacity) ⁇ 100%
- the cut-off current is 0.02C. After 5 minutes of storage, put it at 0.5C to 2.0V, record the initial capacity D1, and then charge it to 3.65V with 0.5C constant current and constant voltage.
- the cut-off current is 0.02C, and the thickness T1, voltage and internal resistance of the battery are tested; after the fully charged battery is stored in a 60°C incubator for 30 days, the thermal thickness of the battery is measured and recorded as T2, and the cold thickness of the battery is tested after leaving it at room temperature for 4 hours.
- Excessive compound represented by structural formula 1 will increase the side reaction inside the battery and increase the battery impedance, which is not conducive to the further improvement of the battery performance; when the content is less than 0.5%, it will form an interface in the negative electrode The membrane is not stable enough, and the performance improvement of lithium iron phosphate battery is not obvious.
- the test results show that the compound represented by structural formula 1 and VC jointly form an interface film on the electrode surface, which improves the migration rate of lithium ions in high-density lithium iron phosphate batteries during high-temperature cycling and reduces the oxidation between the electrolyte solvent and the electrode material.
- the reduction reaction inhibits the formation of lithium dendrites at the anode interface, and finally improves the high-temperature cycling and high-temperature storage performance of lithium iron phosphate batteries.
- ethylene sulfate (DTD) was further added in the non-aqueous electrolyte system of vinylene carbonate (VC) and the compound shown in structural formula 1. ) or methylene methanedisulfonate (MMDS), which further improves the high-temperature cycling performance and high-temperature storage performance of high-compact lithium iron phosphate batteries.
- Example 5 After 1000 cycles of the lithium-ion batteries obtained in Example 5 and Comparative Example 1, disassemble to obtain a negative electrode sheet, and perform SEM imaging. The test structure obtained in Example 5 is shown in Figure 3, and Comparative Example 1 is obtained. The test results are shown in Figure 4.
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Abstract
Description
Claims (10)
- 一种磷酸铁锂电池,其特征在于,包括正极、负极和非水电解液,所述正极包括正极材料层,所述正极材料层的压实密度为2.3~2.8g/cc,所述正极材料层包括正极活性材料,所述正极活性材料包括LiFePO 4;所述非水电解液包括溶剂、电解质盐、碳酸亚乙烯酯和结构式1所示的化合物:A-D-B-E-C结构式1其中,A、B、C各自独立地选自含有环状碳酸酯基、环状硫酸酯基、环状亚硫酸酯基、环状磺酸酯基、环状砜基、环状亚砜基、环状羧酸酯基或环状酸酐基的基团;D、E各自独立地选自单键、或含有亚烃基、醚键、硫氧双键或碳氧双键的基团;以所述非水电解液的总质量为100%计,所述结构式1所示的化合物的添加量为0.01~5%。
- 根据权利要求1所述的磷酸铁锂电池,其特征在于,以所述非水电解液的总质量为100%计,所述碳酸亚乙烯酯的添加量为0.01~5%,更优的,所述碳酸亚乙烯酯的添加量为0.1~2%。
- 根据权利要求1所述的磷酸铁锂电池,其特征在于,所述正极表面通过X-射线光电子能谱法检测,当在284.5eV处获得碳的1s峰时,在162~174eV的区域出现S的特征峰。
- 根据权利要求1所述的磷酸铁锂电池,其特征在于,所述磷酸铁锂电池的充放电电压范围为2.0~3.8V。
- 根据权利要求1所述的磷酸铁锂电池,其特征在于,A、B、C各自独立地含有的环状碳酸酯基、环状硫酸酯基、环状亚硫酸酯基、环状磺酸酯基、环状砜基、环状亚砜基、环状羧酸酯基和环状酸酐基的数量为1~5,且A、B、C含有的环状碳酸酯基、环状硫酸酯基、环状亚硫酸酯基、环状磺酸酯基、环状砜基、环状亚砜基、环状羧酸酯基和环状酸酐基的总数量小于等于10。
- 根据权利要求1-8任一项所述的磷酸铁锂电池,其特征在于,A与C彼此相同,A与B彼此相同或不同,D与E彼此相同。
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CN110931863A (zh) * | 2019-11-12 | 2020-03-27 | 深圳市比克动力电池有限公司 | 电池电解液用添加剂、锂离子电池电解液、锂离子电池 |
CN111628219A (zh) * | 2020-06-05 | 2020-09-04 | 宁德新能源科技有限公司 | 电解液和包含电解液的电化学装置及电子装置 |
CN111755753A (zh) * | 2020-07-09 | 2020-10-09 | 香河昆仑化学制品有限公司 | 一种锂离子电池电解液添加剂环碳酸硫酸乙烯酯及其制备方法 |
CN114068936A (zh) * | 2022-01-14 | 2022-02-18 | 深圳新宙邦科技股份有限公司 | 锂离子电池 |
CN114094109A (zh) * | 2022-01-19 | 2022-02-25 | 深圳新宙邦科技股份有限公司 | 锂离子电池 |
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KR20230148171A (ko) | 2023-10-24 |
US20240194871A1 (en) | 2024-06-13 |
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