CN113054252B - Electrolyte and lithium ion battery - Google Patents
Electrolyte and lithium ion battery Download PDFInfo
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- CN113054252B CN113054252B CN201911372724.8A CN201911372724A CN113054252B CN 113054252 B CN113054252 B CN 113054252B CN 201911372724 A CN201911372724 A CN 201911372724A CN 113054252 B CN113054252 B CN 113054252B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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Abstract
The invention relates to an electrolyte, which comprises lithium salt, an organic solvent and an additive, wherein the additive comprises 0.1-10% of vinylene carbonate, 0.1-5% of fluoroethylene carbonate, 0.1-5% of lithium borate, 0.1-5% of imide lithium salt, 0.1-5% of lithium difluorophosphate, 0.1-2% of a sulfur-containing compound and 50-2000 ppm of hexamethyldisilazane, wherein the total mass of the electrolyte is 100%. According to the invention, by combined use of additives such as vinylene carbonate, fluoroethylene carbonate, lithium borate salt, imide lithium salt, lithium difluorophosphate, sulfur-containing compound, hexamethyldisilazane and the like, a more stable film is formed on the positive electrode and the negative electrode, so that side reaction of the electrolyte and the ternary material under high voltage can be inhibited; meanwhile, the problems of poor circulation, lithium dendrite and the like caused by a thick electrode can be solved.
Description
Technical Field
The invention belongs to the technical field of electrochemistry, and particularly relates to an electrolyte and a lithium ion battery.
Background
In order to meet the requirements of large-scale equipment such as electric bicycles, electric automobiles and the like, lithium ion batteries are required to have high energy density and low cost; from the material point of view, a high-voltage positive electrode material or a high-gram-capacity material needs to be selected; from the design point of view, the content of active substances needs to be increased, and the thickness of the electrode plate needs to be increased.
However, under high voltage, the decomposition of the conventional electrolyte is accelerated by the Ni element, the electrolyte corrodes the positive electrode at high temperature, so that metal ions are dissolved out, and meanwhile, the active substance of the positive electrode is easily reduced and dissolved out under high voltage; the contact distance between active substances at the bottom layer and electrolyte is increased by thickening the pole piece, the migration distance of lithium ions is prolonged, and the wettability and the absorption of the electrolyte are difficult, so that the internal resistance of the battery is large, the polarization is serious, the capacity exertion is abnormal, the rate capability is poor, the lithium precipitation at low temperature and the cycle performance at normal temperature are poor.
Disclosure of Invention
The invention aims to solve the technical problem of providing an electrolyte capable of improving normal-temperature cycle performance and low-temperature lithium dendrite at high voltage and a lithium ion battery.
In order to achieve the purpose, the invention adopts the technical scheme that:
the invention aims to provide an electrolyte, which comprises lithium salt, an organic solvent and an additive, wherein the additive comprises 0.1-10% of vinylene carbonate, 0.1-5% of fluoroethylene carbonate, 0.1-5% of lithium borate, 0.1-5% of imide lithium salt, 0.1-5% of lithium difluorophosphate, 0.1-2% of a sulfur-containing compound and 50-2000 ppm of hexamethyldisilazane, wherein the total mass of the electrolyte is 100%.
Preferably, the lithium borate salt is one or more than two of lithium tetrafluoroborate, lithium bis (oxalato) borate and lithium difluoro (oxalato) borate.
Preferably, the lithium imide salt is one or two of lithium trifluoromethanesulfonylimide and lithium bistrifluoromethylsulfonyl imide.
Preferably, the sulfur-containing compound is allyl sulfate, or a combination of the allyl sulfate and one or more than two of 1, 3-propane sultone, 1,3- (1-propylene) sultone, vinyl sulfite and methylene methane disulfonate.
Further preferably, the sulfur-containing compounds are allyl sulfate and methylene methanedisulfonate.
More preferably, the ratio of the allyl sulfate to the methylene methanedisulfonate is 1: 1-2.
Preferably, the additive comprises 0.1-1% of vinylene carbonate, 0.5-1.5% of fluoroethylene carbonate, 0.5-1.5% of lithium borate, 0.5-2.5% of imide lithium salt, 0.1-1% of lithium difluorophosphate, 0.5-1.5% of sulfur-containing compound and 100-1000 ppm of hexamethyldisilazane.
Preferably, the organic solvent is one or more of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate and propyl methyl carbonate.
More preferably, the organic solvent is a mixed solvent of ethylene carbonate, diethyl carbonate and ethyl methyl carbonate in a volume ratio of 1: 0.9-1.1.
Preferably, the lithium salt is one or more than two of lithium hexafluorophosphate, lithium perchlorate and lithium tetrafluoroborate.
Preferably, the concentration of the lithium salt is 0.5-1.5 mol/L.
A second aspect of the present invention provides a lithium ion battery including a positive electrode, a negative electrode, a separator provided between the positive electrode and the negative electrode, and an electrolyte solution, characterized in that: the electrolyte is the electrolyte.
Preferably, the charge cut-off voltage of the lithium ion battery is greater than 4.2V and less than or equal to 4.5V.
Preferably, the active material of the positive electrode is LiNi x Co y Mn z L (1-x-y-z) O 2 Wherein, L is Al, Sr, Mg, Ti, Ca, Zr, Zn, Si or Fe, x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, and z is more than or equal to 0 and less than or equal to 1.
Preferably, the surface density of the positive pole piece is 40-55 mg/cm 2 The surface density of the negative pole piece is 25-30 mg/cm 2 。
Preferably, the compaction density of the positive pole piece is 3-3.5 g/cm 3 。
Due to the application of the technical scheme, compared with the prior art, the invention has the following advantages:
according to the invention, by combined use of additives such as vinylene carbonate, fluoroethylene carbonate, lithium borate salt, imide lithium salt, lithium difluorophosphate, sulfur-containing compound, hexamethyldisilazane and the like, a more stable film is formed on the positive electrode and the negative electrode, so that side reaction of the electrolyte and the ternary material under high voltage can be inhibited; meanwhile, the problems of poor circulation, lithium dendrite and the like caused by a thick electrode can be solved.
Detailed Description
The present application will be described in detail with reference to examples, but the present application is not limited to these examples. In this specification, "%" represents mass% unless otherwise specified.
Examples 1 to 10
Electrolyte solution: the lithium salt is lithium hexafluorophosphate, the molar concentration of the lithium salt is 1 mol/L, and the solvent is ethylene carbonate: diethyl carbonate: ethyl methyl carbonate ═ 1: 1:1 (volume ratio), other components in the electrolyte and the amount (based on the total mass of the electrolyte) are shown in table 1.
Negative electrode: artificial graphite, positive electrode: 4.4V NCM523 material, wherein the surface density of the positive pole piece is 50mg/cm 2 The compacted density of the positive pole piece is 3.35g/cm 3 (ii) a The surface density of the negative pole piece is 26mg/cm 2 . The electrolyte, the positive electrode and the negative electrode were assembled into a lithium battery according to a conventional process, and the percentage of the capacity of the lithium battery prepared in each example was tested after 500 cycles of charge and discharge at 1C, and the results are shown in table 1. The lithium batteries prepared in the examples were tested for disassembly in a glove box after being charged and discharged for 10 times at-10 ℃ under 0.5C cycle, and the surface of the negative electrode was observed for the presence of lithium dendrites, and the results are shown in table 2.
TABLE 1
TABLE 2
Examples 11 to 19
Electrolyte solution: the lithium salt is lithium hexafluorophosphate, the molar concentration of the lithium salt is 1 mol/L, and the solvent is ethylene carbonate: diethyl carbonate: ethyl methyl carbonate ═ 1: 1:1 (volume ratio), the additive comprises 0.5% of VC, 1% of FEC and 0.5% of LiPO 2 F 2 0.02% HMDS, 1% LiFOB, 1% LiTFSI, other components and amounts in the electrolyte (based on the total mass of the electrolyte) are shown in Table 3.
Negative electrode: artificial graphite, positive electrode: 4.4V NCM523 material, wherein the surface density of the positive pole piece is 50mg/cm 2 The compacted density of the positive pole piece is 3.35g/cm 3 (ii) a The surface density of the negative pole piece is 26mg/cm 2 . The electrolyte, the positive electrode and the negative electrode were assembled into a lithium battery according to a conventional process, and the lithium battery prepared in each example was testedThe results of the percentage of battery capacity after 500 cycles of charge and discharge at 1C are shown in table 3.
TABLE 3
Examples 20 to 22
Electrolyte solution: the lithium salt is lithium hexafluorophosphate, the molar concentration of the lithium salt is 1 mol/L, and the solvent is ethylene carbonate: diethyl carbonate: ethyl methyl carbonate ═ 1: 1:1 (volume ratio), additives including 0.5% VC, 1% FEC, 0.5% MMDS, 0.5% DTD, 0.5% LiPO 2 F 2 0.02% HMDS, 1% LiFOB, other components in the electrolyte and the amounts used (based on the total mass of the electrolyte) are shown in Table 4.
Negative electrode: artificial graphite, positive electrode: 4.4V NCM523 material, wherein the surface density of the positive pole piece is 50mg/cm 2 The compacted density of the positive pole piece is 3.35g/cm 3 (ii) a The surface density of the negative pole piece is 26mg/cm 2 . The electrolyte, the positive electrode and the negative electrode were assembled into a lithium battery according to a conventional process, and the percentage of the capacity of the lithium battery prepared in each example was tested after 500 cycles of charge and discharge at 1C, and the results are shown in table 4.
TABLE 4
Examples 23 to 25
Electrolyte solution: the lithium salt is lithium hexafluorophosphate, the molar concentration of the lithium salt is 1 mol/L, and the solvent is ethylene carbonate: diethyl carbonate: ethyl methyl carbonate ═ 1: 1:1 (volume ratio), additives including 0.5% VC, 1% FEC, 0.5% MMDS, 0.5% DTD, 0.5% LiPO 2 F 2 0.02% HMDS, 1% LiTFSI, other components and amounts in the electrolyte (based on the total mass of the electrolyte) are shown in Table 5.
Negative electrode: artificial graphite, positive electrode: 4.4V NCM523 material, wherein the surface density of the positive pole piece is 50mg/cm 2 The compacted density of the positive pole piece is 3.35g/cm 3 (ii) a The surface density of the negative pole piece is 26mg/cm 2 . The electrolyte, the positive electrode and the negative electrode were assembled into a lithium battery according to a conventional process, and the capacity percentage of the lithium battery prepared in each example was tested after 1C cycle of charge and discharge for 500 times, and the results are shown in table 5.
TABLE 5
| Examples | Borate (%) | Percentage of battery capacity at 25 ℃ (%) |
| 23 | LiFOB(1) | 94 |
| 24 | LiBOB(1) | 85 |
| 25 | LiBF4(1) | 84 |
In the table: VC is vinylene carbonate, FEC is fluoroethylene carbonate, PS is 1, 3-propane sultone, PST is 1,3- (1-propylene) sultone, VES is vinyl ethylene sulfite, DTD is propylene sulfate, MMDS is methylene methane disulfonate, LiPO 2 F 2 Lithium difluorophosphate, LiFSI lithium trifluoromethanesulfonate, LiTFSI lithium bistrifluoromethylsulfonimide, LiBF 4 Is lithium tetrafluoroborate, LiBOB is lithium bis (oxalato) borate, LiFOB is lithium difluoro (oxalato) borate, HMDS is hexamethyl bis (oxalato) borateSilazanes.
The above-mentioned embodiments are provided only for illustrating the technical idea and features of the present invention, and the purpose thereof is to enable those skilled in the art to understand the content of the present invention and to implement the present invention, and not to limit the protection scope of the present invention by this, and all equivalent changes or modifications made according to the spirit of the present invention should be covered in the protection scope of the present invention.
Claims (11)
1. An electrolyte comprising a lithium salt, an organic solvent and an additive, wherein: the electrolyte is characterized in that the total mass of the electrolyte is 100%, the additive comprises 0.1-10% of vinylene carbonate, 0.1-5% of fluoroethylene carbonate, 0.1-5% of lithium borate, 0.1-5% of imide lithium salt, 0.1-5% of lithium difluorophosphate, 0.1-2% of sulfur-containing compounds and 50-2000 ppm of hexamethyldisilazane, the sulfur-containing compounds are allyl sulfate and methylene methane disulfonate, and the electrolyte is used for a lithium ion battery with a thick electrode plate as a positive electrode plate.
2. The electrolyte of claim 1, wherein: the lithium borate salt is one or more than two of lithium tetrafluoroborate, lithium bis (oxalate) borate and lithium difluoro (oxalate) borate.
3. The electrolyte of claim 1, wherein: the imide lithium salt is one or two of trifluoro sulfonyl imide lithium and bis-trifluoro methyl sulfonyl imide lithium.
4. The electrolyte of any one of claims 1 to 3, wherein: the additive comprises 0.1-1% of vinylene carbonate, 0.5-1.5% of fluoroethylene carbonate, 0.5-1.5% of lithium borate, 0.5-2.5% of imide lithium salt, 0.1-1% of lithium difluorophosphate, 0.5-1.5% of sulfur-containing compound and 100-1000 ppm of hexamethyldisilazane.
5. The electrolyte of claim 1, wherein: the organic solvent is one or more than two of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate and propyl methyl carbonate; the lithium salt is one or more than two of lithium hexafluorophosphate, lithium perchlorate and lithium tetrafluoroborate.
6. The electrolyte of claim 5, wherein: the organic solvent is a mixed solvent of ethylene carbonate, diethyl carbonate and ethyl methyl carbonate in a volume ratio of 1: 0.9-1.1; the concentration of the lithium salt is 0.5-1.5 mol/L.
7. A lithium ion battery comprises a positive electrode, a negative electrode, a diaphragm arranged between the positive electrode and the negative electrode, and electrolyte, and is characterized in that: the electrolyte is the electrolyte according to any one of claims 1 to 6.
8. The lithium ion battery of claim 7, wherein: the charge cut-off voltage of the lithium ion battery is greater than 4.2V and less than or equal to 4.5V.
9. The lithium ion battery of claim 7, wherein: the active material of the positive electrode is LiNi x Co y Mn z L (1-x-y-z) O 2 Wherein, L is Al, Sr, Mg, Ti, Ca, Zr, Zn, Si or Fe, x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, and z is more than or equal to 0 and less than or equal to 1.
10. The lithium ion battery of claim 7, wherein: the surface density of the positive pole piece is 40-55 mg/cm 2 The surface density of the negative pole piece is 25-30 mg/cm 2 。
11. The lithium ion battery of claim 7, wherein: the compacted density of the positive pole piece is 3-3.5 g/cm 3 。
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