CN113659210B - 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
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- 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
- 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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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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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 film forming additive accounting for 0.1% -3% 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 the negative electrode material in preference to the solvent, and can be oxidized to form a film on the surface of the positive electrode. Thereby greatly improving the high temperature performance of the lithium ion battery, 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 production.
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 operates mainly by means of lithium ions moving between a positive electrode and a negative electrode. During charge and discharge, li + Back and forth insertion and extraction between the two electrodes; during charging, li + De-intercalation from the positive electrode, and intercalation into the negative electrode through the electrolyte, wherein the negative electrode is in a lithium-rich state; the opposite is true when discharging. 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 aviation, aerospace and the like.The electrolyte is used as a carrier for ion transmission in the lithium ion battery, and plays a vital role in playing various aspects of performances of the lithium ion battery.
Patent CN111564665A discloses an electrolyte of an ultra-high temperature safe lithium ion battery and a lithium ion battery using the electrolyte, wherein the electrolyte 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 disclosed by the invention is a high-temperature solvent and a 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 105261791A discloses an electrolyte for an ultra-high temperature high voltage lithium ion battery and a lithium ion battery using the same. The organic acid catalyst 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 any one or two of lithium fluorosulfonyl imide and cyclic sulfate. According to the invention, the carboxylic ester solvent with high boiling point and good wettability is used for replacing part of the carbonic ester solvent, so that the high-temperature storage performance of the lithium ion battery can be effectively improved, and the wettability of the electrolyte to the graphite negative electrode can be improved.
The lithium ion battery electrolyte material with high temperature resistance is the field which is studied intensively all the time, the high temperature resistance is improved a little bit, along with the development of electrolyte technology, any performance improvement now becomes a step-lifting and difficultly, so the technical problem solved by the scheme is as follows: and developing new high-temperature resistant electrolyte additives, electrolyte and lithium ion batteries.
Disclosure of Invention
In view of the above drawbacks and shortcomings of the prior art, a primary object of the present invention is to provide a high temperature lithium ion battery electrolyte. The electrolyte contains a film forming additive shown in the formula I, which can be reduced to form a film on the surface of the negative electrode material in preference to a solvent, and can be oxidized to form a film on the surface of the positive electrode. The stability of the negative electrode SEI film is ensured, meanwhile, the stability of the positive electrode material can be protected, and the precipitation of active metal elements of the positive electrode is prevented, so that 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 production.
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, the percentages of the present invention are by weight, and M represents mol/L.
The invention aims at realizing the following technical scheme:
the electrolyte of the high-temperature lithium ion battery comprises a film forming additive accounting for 0.1% -3% of the total amount of the electrolyte; the film-forming additive has a structure as shown in formula I:
wherein R is alkyl, aryl, heterocyclic group 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 electrolyte.
Further, the carbonic ester solvent is one or more of propylene carbonate, ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate and diethyl carbonate.
Further, the electrolyte also comprises electrolyte; the electrolyte is one or a combination of a plurality of lithium hexafluorophosphate, lithium bisoxalato borate, lithium bisfluoro sulfonyl imide and lithium bistrifluoromethyl sulfonyl imide; the electrolyte accounts for 5 to 25 percent 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 LiFeSI (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 electrolyte.
Further preferably, the vinylene carbonate, fluoroethylene carbonate, 1, 3-propane sultone and LiFSI respectively account for 0.5 percent, 1 percent to 2 percent, 1 percent and 1.5 percent to 4 percent 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 material 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 a 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 negative electrode SEI film is ensured, meanwhile, the stability of the positive electrode material can be protected, and the precipitation of active metal elements of the positive electrode is prevented, so that 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 production.
Detailed Description
The present invention will be described in further detail with reference to examples, but embodiments of the present invention are not limited thereto.
Examples 1 to 14
The electrolyte compositions of examples 1 to 14 and comparative examples 1 to 2 were designed as shown in table 1 below. Wherein the structures of the compounds 1-5 (N123 additive) are shown in the formula I.
In the compound 1, R is phenyl, and the structure of the compound 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.
Comparative example 1 was not added with the film forming additive of the present invention containing a phenyltriazole structure; compound 6 of comparative example 2 is 3, 5-diphenyl-1-H-1, 2, 4-triazole, which has the structure shown in formula III below.
TABLE 1 electrolyte compositions in examples 1-14 and comparative examples 1-2
The components in the table are described below: EC, ethylene carbonate; EMC, ethyl methyl carbonate; DEC, diethyl carbonate; VC, vinylene carbonate; FEC, fluoroethylene carbonate; PS,1, 3-propane sultone. All are commercial products in the market.
The compounds 1-5 are triazole compounds, the triazole ring is aromatic heterocycle with high stability, the triazole ring cannot be decomposed under acidic and alkaline conditions, and the triazole ring can also show extremely strong stability under redox conditions. At present, a great deal of literature reports that a general method for synthesizing 1H-1,2, 3-triazole is that azide and alkyne compounds are subjected to 1, 3-dipolar cycloaddition reaction, the aromatic trace of 3-benzoyl isoxazole is taken as a starting material, and under the catalysis of copper acetate monohydrate, the reaction is carried out in methanol in a reflux way to generate intramolecular rearrangement reaction, so that the corresponding 2,4, 5-trisubstituted-1, 2, 3-triazole is obtained. Compound 6 is a commercial product.
High temperature lithium ion batteries were prepared according to the electrolyte composition of table 1: and designing 1800mAh according to the capacity of the battery, and determining the coating surface density by the capacity of the anode material and the cathode material. The positive electrode active material is a ternary material purchased from Homehundred S85E; the negative electrode active material is an S360L graphite material purchased from Bei Terui; the membrane was a 20 μm thick PE ceramic membrane purchased from a star source.
The preparation steps of the positive electrode are as follows: positive electrode sheet according to Ni83: CNT: SP: PVDF=97.3:0.5:1:1.2;
the preparation method of the negative electrode comprises the following steps: a negative electrode sheet according to the ratio of C to CMC and SBR=95:1.5:1.5:2;
the preparation method of the electrolyte comprises 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 was 12.5% (1 mol/L) of the total mass of the electrolyte, and the film forming additive and the rest were added.
The lithium ion battery is assembled by the following steps: and winding the positive pole piece, the negative pole piece and the PE ceramic diaphragm to obtain a battery core, putting the battery core into an aluminum plastic film for packaging, drying, injecting electrolyte for sealing, and carrying out the procedures of standing, formation, secondary sealing, capacity division 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, and the test methods were as follows:
1. cycle performance test of lithium ion battery under high temperature condition
45 ℃ 0.5C/0.5C high temperature cycle test: charging to 4.25V at 45deg.C under constant current of 0.5C, charging to cutoff current of 0.05C under constant voltage of 4.25V, discharging the battery with constant current of 0.5C, and recording discharge capacity as C 0 Repeating the charge and discharge steps for 300 weeks to obtain 300 th week discharge capacity C 300 Capacity retention = C 300 /C 0 *100％。
2. Testing of lithium ion batteries in high temperature storage
Cell 60 ℃ 14d storage thickness expansion ratio, capacity retention and capacity recovery test: charging to 4.25V at 25deg.C under constant current of 0.5C, charging to cutoff current of 0.05C under constant voltage of 4.25V, discharging the battery under constant current of 0.5C, and recording discharge capacity as C 0 。
Charging to 4.25V at 25deg.C under constant current and constant voltage of 4.25V to cut-off current of 0.05C, and recording cell thickness D 0 Then the battery is placed in an explosion-proof oven at 60 ℃, and after 14D of storage, the thickness D of the battery is tested in the oven 1 After that, the battery was taken out and cooled to room temperature, and its discharge holding capacity C was measured at 0.5C to 3.0V 2 Then the charge and discharge steps are repeated for 3 weeks, and the discharge capacity C of the battery at the 3 rd week is recorded 3 Thickness expansion ratio= (D) 1 -D 0 )/D 0 *100%, capacity retention = C 2 /C 0 *100%, capacity recovery rate=c 3 /C 0 *100％。
The dcr test method can refer to the procedure of table 2 below:
TABLE 2 DCR test method
The results of the capacity retention rate at 45℃cycle 300 weeks, the capacity recovery rate, the thickness expansion rate and the like of the above examples and comparative examples are shown in Table 3.
TABLE 3 cycle capacity retention, capacity recovery retention, thickness expansion and discharge capacity retention
It can be seen from examples 1 to 9 that: with the increase of the addition amount of the film forming additive N123, the cyclic 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 DCR change rate of 60 ℃ are increased and then reduced under the charge cut-off voltage of 4.25V. The performance is best when the addition amount of N123 is about 1.0%, and the cycle performance of the N123 with the addition amount of 0.5% is obviously better than that of the comparative example when the N123 is compared with the comparative example, and the cycle performance is improved by approximately 8%.
As can be seen from examples 10 to 14: the different structural formulas of the film forming additive N123 have different action effects on the high-temperature cycle performance and the high-temperature storage performance of the battery, and the action effect of the allyl is better than that of the ethynyl > phenyl > alkyl.
As can be seen from example 4 and comparative examples 1 and 2: when 3, 5-diphenyl-1-H-1, 2, 4-triazole additives having no substituent R are used, they contribute to electrical properties, but the electrical effects of the additives of the present invention are not achieved, and referring to Table 3, each of the properties of comparative examples 1 and 2 is inferior to that of example 4, and particularly the DCR growth rate of comparative example is significantly higher than that of example 4.
The above examples are preferred embodiments of the present invention, but the embodiments of the present invention are not limited to the above examples, and any other changes, modifications, substitutions, combinations, and simplifications that do not depart from the spirit and principle of the present invention should be made in the equivalent manner, and the embodiments are included in the protection scope of the present invention.
Claims (8)
1. The high-temperature lithium ion battery electrolyte is characterized in that: the electrolyte contains film forming additive accounting for 0.1% -3% of the total amount of the electrolyte; the film-forming additive has a structure as shown in formula I:
wherein R is allyl, ethynyl or phenyl.
2. The high temperature lithium ion battery electrolyte according to claim 1, wherein: the electrolyte is carbonate-based electrolyte; the carbonate solvent in the carbonate-based electrolyte accounts for 60% -85% of the total electrolyte.
3. The high temperature lithium ion battery electrolyte according to claim 2, wherein: the carbonic ester solvent is one or more of propylene carbonate, ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate and diethyl carbonate.
4. The high temperature lithium ion battery electrolyte according to claim 1, wherein: the electrolyte also comprises electrolyte; the electrolyte is one or a combination of a plurality of lithium hexafluorophosphate, lithium bisoxalato borate, lithium bisfluoro sulfonyl imide and lithium bistrifluoromethyl sulfonyl imide; the electrolyte accounts for 5 to 25 percent of the total amount of the electrolyte.
5. 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 electrolyte.
6. The high temperature lithium ion battery electrolyte according to claim 5, wherein: the vinylene carbonate, fluoroethylene carbonate, 1, 3-propane sultone and LiFSI respectively account for 0.5 percent, 1 percent to 2 percent, 1 percent and 1.5 percent to 4 percent of the total amount of the electrolyte.
7. A lithium ion battery, characterized in that: consists of a positive electrode, a negative electrode, a diaphragm and the high-temperature lithium ion battery electrolyte as claimed in any one of claims 1 to 6.
8. The lithium ion battery of claim 7, wherein: the active material 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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| 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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