CN113659210A - High-temperature lithium ion battery electrolyte and lithium ion battery - Google Patents
High-temperature lithium ion battery electrolyte and lithium ion battery Download PDFInfo
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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
- 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
- H01M10/42—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
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- H—ELECTRICITY
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- 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
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- 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
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Abstract
The invention belongs to the technical field of lithium ion batteries, and discloses a high-temperature lithium ion battery electrolyte and a lithium ion battery. The electrolyte contains a film forming additive which is 0.1 to 3 percent of the total amount of the electrolyte; the film forming additive has a structure shown in a formula I, wherein R is alkyl, aryl, heterocyclic group or unsaturated group. The film forming additive contained in the electrolyte can be reduced to form a film on the surface of a negative electrode material in preference to a solvent, and can be oxidized to form a film on the surface of a positive electrode. Therefore, the high-temperature performance of the lithium ion battery is greatly improved, and the secondary battery containing the additive has good capacity retention rate and capacity recovery rate under the high-temperature condition and can greatly inhibit gas generation.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a high-temperature lithium ion battery electrolyte and a lithium ion battery.
Background
A lithium ion battery is a secondary battery (rechargeable battery) that mainly operates by movement of lithium ions between a positive electrode and a negative electrode. During charging and discharging, Li+Embedding and de-embedding between the two electrodes; upon charging, Li+The lithium ion battery is extracted from the positive electrode and is inserted into the negative electrode through the electrolyte, and the negative electrode is in a lithium-rich state; the opposite is true during discharge. The lithium ion battery has the advantages of high working voltage, large specific capacity, long cycle life, no memory effect, environmental friendliness and the like, and is widely applied to the fields of digital codes, energy storage, power, military aerospace, aviation and the like. The electrolyte is used as a carrier for ion transmission in the lithium ion battery, and plays an important role in playing the performance of the lithium ion battery in all aspects.
Patent CN111564665A discloses an ultra-high temperature safe lithium ion battery electrolyte and a lithium ion battery using the electrolyte, which comprises 10-15% of lithium salt, 1-5% of high temperature film forming additive, 1-10% of flame retardant additive and the balance of organic solvent. The electrolyte is a high-temperature solvent and lithium salt with excellent thermal stability, and a film-forming additive with excellent film-forming thermal stability and a proper flame-retardant additive are added to realize the flame-retardant effect of the electrolyte.
Patent CN 105261791 a discloses an ultrahigh temperature high voltage lithium ion battery electrolyte and a lithium ion battery using the same. The additive comprises a nonaqueous organic solvent, lithium hexafluorophosphate, a gas production inhibiting additive and a low-impedance additive, wherein the nonaqueous organic solvent comprises a carbonate solvent and a high-boiling-point carboxylic ester solvent, and the gas production inhibiting additive is a sultone compound; the low-impedance additive is one or a mixture of two of lithium fluorosulfonyl imide and cyclic sulfate. According to the invention, a part of carbonate solvent is replaced by a carboxylic ester solvent with high boiling point and good wettability, so that the high-temperature storage performance of the lithium ion battery can be effectively improved, and the wettability of the electrolyte on a graphite cathode can be improved.
High temperature resistant lithium ion battery electrolyte material is the field of focus research all the time, and everybody is at the improvement high temperature resistance performance of a bit, and along with the development of electrolyte technique, the improvement of any performance has become to hold step hard now, so, the technical problem that the present case was solved is: how to develop a new high-temperature-resistant electrolyte additive, an electrolyte and a lithium ion battery.
Disclosure of Invention
Aiming at the defects and shortcomings of the prior art, the invention mainly aims to provide a high-temperature lithium ion battery electrolyte. The electrolyte contains a film forming additive shown as a formula I, can be reduced to form a film on the surface of a negative electrode material in preference to a solvent, and can be oxidized to form a film on the surface of a positive electrode. The stability of the SEI film of the negative electrode can be ensured, the stability of the positive electrode material can be protected, the active metal elements of the positive electrode can be prevented from being separated out, the high-temperature performance of the lithium ion battery can be greatly improved, the secondary battery containing the additive has good capacity retention rate and capacity recovery rate under the high-temperature condition, and the gas generation can be greatly inhibited.
Another object of the present invention is to provide a lithium ion battery. The lithium ion battery comprises the high-temperature lithium ion battery electrolyte.
Unless otherwise specified,% of the present invention represents weight percent, and M represents mol/L.
The purpose of the invention is realized by the following technical scheme:
the electrolyte of the high-temperature lithium ion battery contains a film forming additive which is 0.1 to 3 percent of the total amount of the electrolyte; the film-forming additive has a structure as shown in formula I below:
wherein R is alkyl, aryl, heterocyclic radical or unsaturated group.
Further, R is C1-C6 alkyl, phenyl, C5-C12 heterocyclic group, vinyl, allyl, ethynyl or acetonitrile.
Further preferably, R is allyl, ethynyl, or phenyl.
Further, the electrolyte is a carbonate-based electrolyte.
Further, the carbonate solvent in the carbonate-based electrolyte accounts for 60-85% of the total amount of the electrolyte.
Further, the carbonate solvent is one or more of propylene carbonate, ethylene carbonate, ethyl methyl carbonate, dimethyl carbonate and diethyl carbonate.
Further, the electrolyte also comprises an electrolyte; the electrolyte is one or a combination of more of lithium hexafluorophosphate, lithium bis (oxalato) borate, lithium bis (fluorosulfonyl) imide and lithium bis (trifluoromethylsulfonyl) imide; the electrolyte accounts for 5-25% of the total amount of the electrolyte. Experiments prove that the change of the electrolyte dosage does not have fundamental influence on the performance trend of the scheme.
Further, the electrolyte also comprises an auxiliary additive; the auxiliary additive is one or a combination of more of vinylene carbonate, fluoroethylene carbonate, 1, 3-propane sultone and LiFSI (lithium bis (fluorosulfonyl imide)), wherein the vinylene carbonate, the fluoroethylene carbonate and the 1, 3-propane sultone respectively account for 0-3% of the total amount of the electrolyte; LiFSI accounts for 0% -4% of the total amount of the electrolyte.
More preferably, the vinylene carbonate, the fluoroethylene carbonate, the 1, 3-propane sultone and the LiFSI respectively account for 0.5%, 1% -2%, 1% and 1.5-4% of the total amount of the electrolyte.
A lithium ion battery consists of a positive electrode, a negative electrode, a diaphragm and the high-temperature lithium ion battery electrolyte.
Further, the active substance of the positive electrode is a ternary material, and the negative electrode is one or two of graphite and silicon carbon.
Compared with the prior art, the invention has the beneficial effects that:
the electrolyte contains the film forming additive shown in the formula I, can be reduced to form a film on the surface of a negative electrode material in preference to a solvent, and can be oxidized to form a film on the surface of a positive electrode. The stability of the SEI film of the negative electrode can be ensured, the stability of the positive electrode material can be protected, the active metal elements of the positive electrode can be prevented from being separated out, the high-temperature performance of the lithium ion battery can be greatly improved, the secondary battery containing the additive has good capacity retention rate and capacity recovery rate under the high-temperature condition, and the gas generation can be greatly inhibited.
Detailed Description
The present invention will be described in further detail with reference to examples, but the embodiments of the present invention are not limited thereto.
Examples 1 to 14
The compositions of the electrolytes of examples 1 to 14 and comparative examples 1 to 2 were designed as shown in Table 1 below. The structure of the compound 1-5 (N123 additive) is shown as a formula I.
In the compound 1, R is phenyl, and the structure of the R is shown as the following formula II:
r in the compound 2 is methyl; r in the compound 3 is propyl; r in the compound 4 is ethynyl; in the compound 5, R is allyl.
In the comparative example 1, the film forming additive containing the phenyl triazole structure is not added; in comparative example 2, compound 6 is 3, 5-diphenyl-1-H-1, 2, 4-triazole, and the structure is shown in formula III below.
TABLE 1 electrolyte compositions of examples 1 to 14 and comparative examples 1 to 2
The ingredients in the table are illustrated below: EC, ethylene carbonate; EMC, ethyl methyl carbonate; DEC, diethyl carbonate; VC, vinylene carbonate; FEC, fluoroethylene carbonate; PS, 1, 3-propane sultone. Are all market commercial products.
The compounds 1-5 are triazole compounds, and the triazole ring is a high-stability aromatic heterocyclic ring, cannot be decomposed under acidic and alkaline conditions, and can show extremely high stability under redox conditions. At present, a large number of documents report that the general method for synthesizing 1H-1,2, 3-triazole is a dipolar cycloaddition reaction of azide and acetylene compounds 1,3, and the aromatic trace of 3-benzoyl isoxazole is used as a starting material, and is refluxed in methanol under the catalysis of copper acetate monohydrate to generate an intramolecular rearrangement reaction, so that the corresponding 2,4, 5-trisubstituted-1, 2, 3-triazole is obtained. Compound 6 is a commercial product.
A high temperature lithium ion battery was prepared with the electrolyte composition of table 1: and determining the coating surface density according to the capacity design 1800mAh and the capacities of the anode and cathode materials of the battery. The positive active material is a ternary material purchased from hundreds of S85E; the negative active material is S360L graphite material from fibrate; the diaphragm is a PE ceramic diaphragm which is purchased from a star source and has the thickness of 20 mu m.
The preparation steps of the anode are as follows: a positive electrode sheet comprising Ni83, CNT, SP, PVDF, 97.3:0.5:1: 1.2;
the preparation steps of the negative electrode are as follows: a negative plate with the weight ratio of C, SP, CMC, SBR to 95:1.5:1.5: 2;
the electrolyte is prepared by the following steps: in a glove box filled with argon, EC, EMC and DEC were mixed in the weight ratio of table 1, the mass percentage of the solvent was 85% of the total mass of the electrolyte, lithium hexafluorophosphate was used as the lithium salt, the mass percentage thereof was 12.5% (1mol/L) of the total mass of the electrolyte, and the film forming additive and the rest of the additives were added.
The lithium ion battery assembling steps are as follows: and winding the positive pole piece, the negative pole piece and the PE ceramic diaphragm to obtain a battery core, placing the battery core into an aluminum plastic film for packaging, drying, injecting an electrolyte for sealing, standing, forming, secondary sealing, capacity grading and the like to obtain the lithium ion battery.
The lithium ion batteries obtained in the above examples and comparative examples were subjected to performance tests, the test methods were as follows:
1. cycle performance test of lithium ion battery under high temperature condition
High temperature cycle test at 45 ℃ 0.5C/0.5C: charging to 4.25V at 45 deg.C under constant current of 0.5C and constant voltage of 4.25V to 0.05C at cut-off current, and discharging at constant current of 0.5C to obtain discharge capacity C0Repeating the charging and discharging steps for 300 weeks to obtain the discharge capacity C at 300 th week300Capacity retention rate ═ C300/C0*100％。
2. Testing of lithium ion batteries at high temperature storage
Battery 60 ℃ 14d storage thickness expansion ratio, capacity retention and capacity recovery test: charging to 4.25V at 25 deg.C under constant current of 0.5C and constant voltage of 4.25V to 0.05C at cut-off current, and discharging at constant current of 0.5C to obtain discharge capacity C0。
Charging at 25 deg.C and constant current of 0.5C to 4.25V, charging at constant voltage of 4.25V to cutoff current of 0.05C, and recording the thickness D of the battery0Then the battery is placed in an explosion-proof oven at 60 ℃, and after being stored for 14D, the thickness D of the battery is tested in the oven1Then, the cell was taken out and cooled to room temperature, and the discharge retention capacity C of 0.5C-discharge to 3.0V was tested2Then repeating the charging and discharging steps for 3 weeks, and recording the 3 rd week discharge capacity C of the battery3Thickness expansion ratio ═ D1-D0)/D0100%, capacity retention ═ C2/C0100%, capacity recovery rate ═ C3/C0*100％。
DCR test method, reference is made to the procedure of table 2 below:
TABLE 2 DCR test method
The results of the capacity retention ratio at 45 ℃ for 300 weeks and the capacity retention ratio, the capacity recovery ratio, the thickness expansion ratio and the like at 60 ℃ for 14 days in the examples and comparative examples are shown in Table 3.
TABLE 3 retention ratio of cyclic capacity, retention ratio of capacity recovery rate, thickness expansion rate and retention ratio of discharge capacity
The following examples 1 to 9 show that: with the increase of the addition amount of the film forming additive N123, 0.1% -3%, under the charge cut-off voltage of 4.25V, the cycle capacity retention rate of 45 ℃ 1C, the high-temperature storage capacity retention rate of 60 ℃, the high-temperature storage thickness expansion rate of 60 ℃ and the change rate of DCR stored at 60 ℃ show the trend of increasing and then decreasing. The performance is best when the addition amount of the N123 is about 1.0 percent, and compared with a comparative example, the cycle performance at 45 ℃ is obviously better than that of the comparative example and the cycle performance is improved by nearly 8 percent when the N123 with 0.5 percent is added.
As can be seen from examples 10 to 14: the different structural formulas of the film forming additive N123 have different effects on the high-temperature cycle performance and the high-temperature storage performance of the battery, and the effect of allyl is superior to that of ethynyl > phenyl > alkyl.
As can be seen from example 4 and comparative examples 1 and 2: when the 3, 5-diphenyl-1-H-1, 2, 4-triazole additive without the substituent group R is adopted, certain contribution is made to the electrical property, but the electrical effect of the additive disclosed by the invention cannot be achieved, referring to the table 3, the properties of comparative examples 1 and 2 are inferior to those of example 4, and particularly the DCR growth rate of the comparative examples is obviously higher than that of example 4.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.
Claims (10)
1. The high-temperature lithium ion battery electrolyte is characterized in that: the electrolyte contains a film forming additive which is 0.1 to 3 percent of the total amount of the electrolyte; the film-forming additive has a structure as shown in formula I below:
wherein R is alkyl, aryl, heterocyclic radical or unsaturated group.
2. The high-temperature lithium ion battery electrolyte according to claim 1, wherein: and R is C1-C6 alkyl, phenyl, C5-C12 heterocyclic group, vinyl, allyl, ethynyl or acetonitrile.
3. The high-temperature lithium ion battery electrolyte according to claim 1, wherein: and R is allyl, ethynyl or phenyl.
4. The high-temperature lithium ion battery electrolyte according to claim 1, wherein: the electrolyte is a carbonate-based electrolyte; the carbonate solvent in the carbonate-based electrolyte accounts for 60-85% of the total amount of the electrolyte.
5. The high-temperature lithium ion battery electrolyte according to claim 4, wherein: the carbonate solvent is one or more of propylene carbonate, ethylene carbonate, ethyl methyl carbonate, dimethyl carbonate and diethyl carbonate.
6. The high-temperature lithium ion battery electrolyte according to claim 1, wherein: the electrolyte also comprises an electrolyte; the electrolyte is one or a combination of more of lithium hexafluorophosphate, lithium bis (oxalato) borate, lithium bis (fluorosulfonyl) imide and lithium bis (trifluoromethylsulfonyl) imide; the electrolyte accounts for 5-25% of the total amount of the electrolyte.
7. The high-temperature lithium ion battery electrolyte according to claim 1, wherein: the electrolyte also comprises an auxiliary additive; the auxiliary additive is one or a combination of more of vinylene carbonate, fluoroethylene carbonate, 1, 3-propane sultone and LiFSI, wherein the vinylene carbonate, the fluoroethylene carbonate and the 1, 3-propane sultone respectively account for 0-3% of the total amount of the electrolyte; LiFSI accounts for 0% -4% of the total amount of the electrolyte.
8. The high temperature lithium ion battery electrolyte of claim 7, wherein: the vinylene carbonate, the fluoroethylene carbonate, the 1, 3-propane sultone and the LiFSI respectively account for 0.5 percent, 1 percent to 2 percent, 1 percent and 1.5 to 4 percent of the total amount of the electrolyte.
9. A lithium ion battery, characterized by: the electrolyte consists of a positive electrode, a negative electrode, a separator and the high-temperature lithium ion battery electrolyte as claimed in any one of claims 1 to 8.
10. A lithium ion battery according to claim 9, wherein: the active substance of the positive electrode is a ternary material, and the negative electrode is one or two of graphite and silicon carbon.
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| TW200605426A (en) * | 2004-05-12 | 2006-02-01 | Mitsui Mining & Smelting Co | Negative electrode for nonaqueous secondary battery and process of producing the same |
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| CN108598488A (en) * | 2018-06-08 | 2018-09-28 | 东莞市杉杉电池材料有限公司 | A kind of lithium ion battery with high energy density and its electrolyte |
| CN110391457A (en) * | 2018-04-23 | 2019-10-29 | 宁德时代新能源科技股份有限公司 | Electrolyte and lithium ion battery |
| CN111200162A (en) * | 2019-12-06 | 2020-05-26 | 联动天翼新能源有限公司 | Lithium ion battery electrolyte and preparation method thereof |
| CN112510262A (en) * | 2020-12-04 | 2021-03-16 | 广州天赐高新材料股份有限公司 | High-temperature lithium ion battery electrolyte and lithium ion battery |
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Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TW200605426A (en) * | 2004-05-12 | 2006-02-01 | Mitsui Mining & Smelting Co | Negative electrode for nonaqueous secondary battery and process of producing the same |
| CN104610288A (en) * | 2015-02-26 | 2015-05-13 | 天津师范大学 | Phenyl triazole silver complex serving as potential fluorescent material and preparation method of phenyl triazole silver complex |
| CN110391457A (en) * | 2018-04-23 | 2019-10-29 | 宁德时代新能源科技股份有限公司 | Electrolyte and lithium ion battery |
| CN108598488A (en) * | 2018-06-08 | 2018-09-28 | 东莞市杉杉电池材料有限公司 | A kind of lithium ion battery with high energy density and its electrolyte |
| CN111200162A (en) * | 2019-12-06 | 2020-05-26 | 联动天翼新能源有限公司 | Lithium ion battery electrolyte and preparation method thereof |
| CN112510262A (en) * | 2020-12-04 | 2021-03-16 | 广州天赐高新材料股份有限公司 | High-temperature lithium ion battery electrolyte and lithium ion battery |
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