CN114094183A - Electrolyte and application thereof - Google Patents
Electrolyte and application thereof Download PDFInfo
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- CN114094183A CN114094183A CN202111321627.3A CN202111321627A CN114094183A CN 114094183 A CN114094183 A CN 114094183A CN 202111321627 A CN202111321627 A CN 202111321627A CN 114094183 A CN114094183 A CN 114094183A
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- electrolyte
- carbonate
- lithium
- ion battery
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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
- 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
- H01M10/0568—Liquid materials characterised by the solutes
-
- 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
- H01M2300/0028—Organic electrolyte characterised by the solvent
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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
Abstract
The invention provides an electrolyte and application thereof, wherein the electrolyte comprises a non-aqueous solvent, a lithium salt and an additive, the additive comprises tetraethoxysilane and vinylene carbonate, and the tetraethoxysilane and the vinylene carbonate are added into the electrolyte, so that the cycle and storage performances of a battery at a high temperature of 45-60 ℃ can be improved.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and relates to an electrolyte and application thereof.
Background
In recent years, new energy electric vehicles and energy storage services have been rapidly increased along with the global market demands and the guidance of policy and regulation; as one of the main technical routes of the cell chemical system, the lithium iron phosphate material occupies a higher market share by virtue of lower cost, wider source and higher safety characteristic. In particular, the low cost and high safety feature make it popular in the energy storage industry.
The energy storage battery cell is influenced by the use environment, the working temperature can exceed more than 45 ℃ when the energy storage battery cell is used in a high-heat area and generates heat, and the service life of the battery cell is shortened sharply when the battery cell is used circularly in the period.
The development of the electrolyte which has both the cycle performance and the storage performance at the high temperature of 45-60 ℃ is necessary.
Disclosure of Invention
The invention aims to provide an electrolyte and application thereof, and the electrolyte is added with tetraene silane and vinylene carbonate, so that the cycle and storage performance of a battery at a high temperature of 45-60 ℃ can be improved.
In order to achieve the purpose, the invention adopts the following technical scheme:
compared with the prior art, the invention has the following beneficial effects:
in a first aspect, the present invention provides an electrolyte comprising a non-aqueous solvent, a lithium salt and an additive comprising Tetraethenylsilane (TVSi) and Vinylene Carbonate (VC).
According to the invention, tetraene silane and vinylene carbonate are added into the electrolyte, so that the performance of the electrolyte at 45-60 ℃ is improved, wherein VC serving as a traditional additive can improve the cycle and high-temperature performance; by adding TVSi, the TVSi contains more unsaturated double bonds, unstable free radicals in electrolyte can be absorbed, side reactions are reduced, electrons are generated on the surface of the cathode to generate organic carbonate to protect the cathode, and therefore high-temperature circulation and storage characteristics are improved.
Preferably, the non-aqueous solvent comprises any one of dimethyl carbonate, ethylmethyl carbonate, ethylene carbonate, propylene carbonate or diethyl carbonate or a combination of at least two thereof.
Preferably, the non-aqueous solvent includes ethylene carbonate, ethylmethyl carbonate and dimethyl carbonate.
Preferably, the mass ratio of the Ethylene Carbonate (EC), the Ethyl Methyl Carbonate (EMC), the dimethyl carbonate (DMC) and the Propylene Carbonate (PC) is (1-5): 2-7): 1-6): 0-4, for example: 1:2:3:0, 1:5:4:2, 2:6:4:3, 3:7:5: 3 or 5:7:6:1, etc.
Preferably, the lithium salt comprises any one of lithium hexafluorophosphate, lithium difluorophosphate or lithium bis-fluorosulfonylimide or a combination of at least two thereof.
Preferably, the mass concentration of the lithium salt is 10-15%, for example: 10%, 11%, 12%, 13%, 14%, 15%, etc.
Preferably, the mass fraction of the tetraethylene silane is 0.01-1% based on 100% of the electrolyte, such as: 0.01%, 0.05%, 0.1%, 0.2%, 0.3%, 0.5%, 1%, or the like.
If the addition amount of the tetraene silane is too small, the high-temperature performance of the electrolyte is not obviously improved, and if the addition amount of the tetraene silane is too large, the resistance of the battery cell is large due to the fact that the resistance of the battery cell is large, so that the performance is deteriorated.
Preferably, the vinylene carbonate accounts for 0.1-3% of the electrolyte by weight, for example: 0.1%, 0.5%, 1%, 1.5%, 2%, or 3%, etc.
Preferably, the mass ratio of the tetraethylene silane to the vinylene carbonate is 1 (10-30), such as: 1:10, 1:15, 1:20, 1:25, 1:30, etc.
If the concentration of the vinylene carbonate is too low, the high-temperature cycle performance of the electrolyte cannot be obviously improved, and if the concentration of the vinylene carbonate is too high, the recovery rate of the high-temperature storage capacity of the electrolyte is obviously reduced.
In a second aspect, the present invention provides a lithium ion battery comprising the electrolyte according to the first aspect.
Preferably, the lithium ion battery further comprises a positive electrode, a negative electrode and a separator.
Preferably, the active material of the positive electrode comprises any one of lithium iron phosphate, lithium cobaltate, lithium manganate or ternary nickel cobalt manganese material or a combination of at least two of the materials.
Preferably, the active material of the negative electrode includes any one of crystalline carbon, amorphous carbon, a carbon composite material, natural graphite, or artificial graphite, or a combination of at least two thereof.
Preferably, the separator comprises a PP/PE/PP separator.
Compared with the prior art, the invention has the following beneficial effects:
(1) according to the invention, tetraene silane and vinylene carbonate are added into the electrolyte, so that the performance of the electrolyte at 45-60 ℃ is improved, wherein VC serving as a traditional additive can improve the cycle and high-temperature performance; by adding TVSi, the TVSi contains more unsaturated double bonds, unstable free radicals in electrolyte can be absorbed, side reactions are reduced, electrons are obtained on the surface of the negative electrode to generate organic carbonate to protect the negative electrode, and therefore high-temperature circulation and storage characteristics are improved.
(2) The capacity retention rate of a battery prepared by using the electrolyte can reach more than 56% at 45 ℃ after 1000 cycles, can reach more than 61.1% at 55 ℃ after 800 cycles, can reach more than 63.4% at 60 ℃, and can reach more than 76.4% of high-temperature storage capacity recovery rate, and the capacity retention rate of the battery can reach 91% at 45 ℃ after 1000 cycles, 87.7% at 55 ℃ after 800 cycles, 83.5% at 60 ℃ after 800 cycles, and 96.4% at high-temperature storage capacity recovery rate by adjusting the mass fractions of tetraethynylsilane and vinylene carbonate in the electrolyte.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments. It should be understood by those skilled in the art that the examples are only for the understanding of the present invention and should not be construed as the specific limitations of the present invention.
In the prior art, a technical scheme provides a high-compaction lithium iron phosphate lithium ion battery non-aqueous electrolyte and a lithium ion battery. The non-aqueous electrolyte comprises a non-aqueous organic solvent, an electrolyte lithium salt and additives, wherein the additives comprise conventional additives and fluoroether additives. The additive in the non-aqueous electrolyte has good wettability and oxidation resistance, and can effectively solve the problems that the high-compaction lithium iron phosphate lithium ion battery has insufficient liquid absorption amount and overlong activation time of a pole piece and a diaphragm due to overlarge compaction density of a positive pole piece and a negative pole piece, so that the cycle performance, the high-temperature storage performance, the low-temperature discharge performance and the production efficiency of the lithium iron phosphate battery are influenced. But the circulation performance of the electrolyte is obviously reduced under the condition of high temperature of more than 45 ℃.
Another aspect provides a nonaqueous electrolyte for a battery for a lithium secondary battery containing lithium iron phosphate as a positive electrode active material, the nonaqueous electrolyte for a battery containing a compound represented by formula (1). In the formula (1), R11 and R12 each independently represent an aliphatic group having 1 to 12 carbon atoms or a fluoroaliphatic group having 1 to 12 carbon atoms. R11-N-C-N-R12 (1). The high-temperature storage performance of the electrolyte is poor.
The electrolyte prepared by the scheme has the problem of poor cycle performance or poor storage performance under a high-temperature condition.
In order to solve at least the technical problems, the invention provides an electrolyte and application thereof, wherein the electrolyte comprises a non-aqueous solvent, a lithium salt and an additive, the additive comprises tetraethenylsilane and vinylene carbonate, and the tetraethenylsilane and vinylene carbonate are added into the electrolyte, so that the cycle and storage performance of the battery at a high temperature of 45-60 ℃ can be improved.
In the embodiment of the disclosure, the electrolyte comprises a non-aqueous solvent, a lithium salt and an additive, wherein the additive comprises tetravinylsilane and vinylene carbonate, and the tetravinylsilane and the vinylene carbonate are added into the electrolyte to improve the performance of the electrolyte at 45-60 ℃, wherein VC is used as a traditional additive to improve the cycle and high-temperature performance; the high-temperature cycle and storage performance can be obviously improved by adding TVSi.
Example 1
The embodiment provides an electrolyte, and the electrolyte comprises the following components: mixing the EC/EMC/DMC components in a ratio of about 3:4:3 into a non-aqueous organic solvent, and mixing with 14 wt% LiPF6After mixing, and the mass fraction of tetraethenylsilane was 0.1% with respect to 100 parts by weight of the nonaqueous electrolyte solution, and that of vinylene carbonateThe mass fraction is 2%.
Example 2
The embodiment provides an electrolyte, and the electrolyte comprises the following components: mixing the components of EC/EMC/DMC/PC in a ratio of about 3:4:3:2 to form a non-aqueous organic solvent, and mixing with 12 wt% LiPF6After the mixing, and with respect to 100 parts by weight of the nonaqueous electrolyte solution, the mass fraction of tetraethoxysilane was 0.2%, and the mass fraction of vinylene carbonate was 2.5%.
Example 3
The embodiment provides an electrolyte, and the electrolyte comprises the following components: mixing the EC/EMC/DMC components in a ratio of about 3:4:3 into a non-aqueous organic solvent, and mixing with 14 wt% LiPF6After the mixing, the mass fraction of tetraethenylsilane was 0.005% and the mass fraction of vinylene carbonate was 2% with respect to 100 parts by weight of the nonaqueous electrolyte solution.
Example 4
Mixing the EC/EMC/DMC components in a ratio of about 3:4:3 into a non-aqueous organic solvent, and mixing with 14 wt% LiPF6After the mixing, and with respect to 100 parts by weight of the nonaqueous electrolyte solution, the mass fraction of tetraethoxysilane was 1.5%, and the mass fraction of vinylene carbonate was 2%.
Example 5
Mixing the EC/EMC/DMC components in a ratio of about 3:4:3 into a non-aqueous organic solvent, and mixing with 14 wt% LiPF6After the mixing, and with respect to 100 parts by weight of the nonaqueous electrolyte solution, the mass fraction of tetraethoxysilane was 0.1%, and the mass fraction of vinylene carbonate was 0.05%.
Example 6
Mixing the EC/EMC/DMC components in a ratio of about 3:4:3 into a non-aqueous organic solvent, and mixing with 14 wt% LiPF6After the mixing, the mass fraction of tetraethenylsilane was 0.1% and the mass fraction of vinylene carbonate was 4% with respect to 100 parts by weight of the nonaqueous electrolyte solution.
Comparative example 1
Mixing the EC/EMC/DMC components in a ratio of about 3:4:3 into a non-aqueous organic solvent, and mixing with 14 wt% LiPF6After the mixing, and with respect to 100 parts by weight of the nonaqueous electrolyte solution, no tetraethylene silane was added, and the mass fraction of vinylene carbonate was 4%.
Comparative example 2
Mixing the EC/EMC/DMC components in a ratio of about 3:4:3 into a non-aqueous organic solvent, and mixing with 14 wt% LiPF6After the mixing, the mass fraction of tetraethenylsilane was 0.1% with respect to 100 parts by weight of the nonaqueous electrolyte solution, and vinylene carbonate was not added.
And (3) performance testing:
lithium iron phosphate 97 wt% as a positive electrode active material, carbon black 2 wt% as a conductive agent, and PVDF 1 wt% as a binder were added to NMP as a solvent to prepare a positive electrode mixture slurry. Coating the positive electrode mixture slurry on an aluminum foil with a thickness of about 15um as a positive electrode current collector, drying, and then performing roll-in die-cutting on the aluminum foil to obtain a positive electrode;
a negative electrode mixture slurry was prepared by dissolving 98 wt% artificial graphite as a negative electrode active material, 1 wt% SBR as a binder, and 1 wt% CMC as a thickener in water. Coating the negative electrode mixture slurry on copper foil with the thickness of 8um serving as a negative electrode current collector, drying, and then rolling and die-cutting the copper foil to obtain a negative electrode;
the positive and negative electrodes were manufactured into laminate pouch batteries together with a separator formed of three PP/PE/PP in a conventional method, after which the non-aqueous electrolyte solutions prepared in examples 1 to 6 and comparative examples 1 to 2 were injected and the preparation of lithium secondary batteries was completed.
The lithium secondary battery is circulated under the environment of 45 ℃, 55 ℃ and 60 ℃, and the capacity retention rate is measured, the voltage interval is 2.5V-3.65V, and the charge-discharge multiplying power is 1C/1C; storing the product for 30d in an environment at 60 ℃, measuring the recovery rate of the cell capacity, and the test result is shown in table 1:
TABLE 1
As can be seen from table 1, in examples 1 to 6, the capacity retention rate of the battery manufactured by using the electrolyte of the present invention can reach more than 56% at 45 ℃ for 1000 cycles, can reach more than 61.1% at 55 ℃ for 800 cycles, can reach more than 63.4% at 60 ℃ for 800 cycles, and can reach more than 76.4% of the high-temperature storage capacity recovery rate, by adjusting the mass fractions of tetraenylsilane and vinylene carbonate in the electrolyte, the capacity retention rate of the battery manufactured at 45 ℃ for 1000 cycles can reach 91%, the capacity retention rate at 55 ℃ for 800 cycles can reach 87.7%, the capacity retention rate at 60 ℃ for 800 cycles can reach 83.5%, and the high-temperature storage capacity recovery rate can reach 96.4%.
Compared with the embodiment 1 and the embodiments 3 to 4, the quality fraction of the tetraene silane in the electrolyte can influence the performance of the electrolyte, the quality fraction of the tetraene silane in the electrolyte is controlled to be 0.01-1%, the prepared electrolyte can give consideration to both the high-temperature cycle performance and the high-temperature storage capacity recovery rate of the electrolyte, if the addition amount of the tetraene silane is too small, the high-temperature performance of the electrolyte is not obviously improved, and if the addition amount of the tetraene silane is too large, the cell impedance is large due to the fact that the resistance of the cell is large, so that the performance is deteriorated.
Compared with the examples 5 to 6, the electrolyte prepared by controlling the mass fraction of the vinylene carbonate in the electrolyte to be 0.1-3% can take the high-temperature cycle performance and the high-temperature storage capacity recovery rate of the electrolyte into consideration, if the concentration of the vinylene carbonate is too low, the high-temperature cycle performance of the electrolyte cannot be obviously improved, and if the concentration of the vinylene carbonate is too high, the high-temperature storage capacity recovery rate of the electrolyte is obviously reduced.
Compared with the comparative example 1, the invention has the advantages that by adding TVSi, the TVSi contains more unsaturated double bonds, unstable free radicals in the electrolyte can be absorbed, side reactions are reduced, electrons are obtained on the surface of the cathode to generate organic carbonate to protect the cathode, so that the high-temperature cycle and storage characteristics are improved, and the high-temperature cycle and storage can be obviously improved by less addition amount compared with VC.
Compared with the comparative example 1 and the comparative example 2, the electrolyte prepared by adding the vinylene carbonate can improve the circulation and high-temperature performance of the electrolyte, and the vinylene carbonate is changed into other carbonate compounds, so that the performance of the electrolyte is obviously poor, and the vinylene carbonate can cooperate with TVSi to ensure the high-temperature circulation performance of the electrolyte and also give consideration to the high-temperature storage performance of the electrolyte.
The applicant declares that the above description is only a specific embodiment of the present invention, but the scope of the present invention is not limited thereto, and it should be understood by those skilled in the art that any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are within the scope and disclosure of the present invention.
Claims (10)
1. An electrolyte comprising a non-aqueous solvent, a lithium salt and an additive, wherein the additive comprises tetravinylsilane and vinylene carbonate.
2. The electrolyte of claim 1, wherein the non-aqueous solvent comprises any one of dimethyl carbonate, ethylmethyl carbonate, ethylene carbonate, propylene carbonate, or diethyl carbonate, or a combination of at least two thereof;
preferably, the non-aqueous solvent comprises ethylene carbonate, ethylmethyl carbonate and dimethyl carbonate;
preferably, the mass ratio of the ethylene carbonate, the ethyl methyl carbonate, the dimethyl carbonate and the propylene carbonate is (1 to 5): (2 to 7): (1 to 6): (0 to 4).
3. The electrolyte of claim 1 or 2, wherein the lithium salt comprises any one of lithium hexafluorophosphate, lithium difluorophosphate or lithium bis-fluorosulfonylimide or a combination of at least two thereof;
preferably, the lithium salt is present in a mass concentration of 10% to 15%.
4. The electrolyte of any one of claims 1 to 3, wherein the mass fraction of the tetravinylsilane is 0.01% to 1%, based on 100% by mass of the electrolyte;
preferably, the vinylene carbonate accounts for 0.1-3% of the electrolyte by mass.
5. The electrolyte of any one of claims 1 to 4, wherein the mass ratio of the tetraethylene silane to the vinylene carbonate is 1 (10 to 30).
6. A lithium ion battery comprising the electrolyte of any one of claims 1 to 5.
7. The lithium ion battery of claim 6, further comprising a positive electrode, a negative electrode, and a separator.
8. The lithium ion battery of claim 7, wherein the active material of the positive electrode comprises any one of lithium iron phosphate, lithium cobaltate, lithium manganate or ternary nickel cobalt manganese materials or a combination of at least two thereof.
9. The lithium ion battery according to claim 7, wherein the active material of the negative electrode comprises any one of crystalline carbon, amorphous carbon, a carbon composite, natural graphite, or artificial graphite, or a combination of at least two thereof.
10. The lithium ion battery of claim 7, wherein the separator comprises a PP/PE/PP separator.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116344916A (en) * | 2023-05-29 | 2023-06-27 | 宁德时代新能源科技股份有限公司 | Lithium secondary battery and electricity utilization device |
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| CN112531212A (en) * | 2020-12-09 | 2021-03-19 | 远景动力技术(江苏)有限公司 | Non-aqueous electrolyte with high-temperature characteristic and low impedance, application thereof and lithium ion battery |
| CN113161613A (en) * | 2021-04-19 | 2021-07-23 | 杉杉新材料（衢州）有限公司 | Lithium ion battery non-aqueous electrolyte and lithium ion battery |
| CN113161615A (en) * | 2021-06-04 | 2021-07-23 | 湖州昆仑亿恩科电池材料有限公司 | Non-aqueous electrolyte of lithium ion battery and lithium ion battery |
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- 2021-11-09 CN CN202111321627.3A patent/CN114094183A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112531212A (en) * | 2020-12-09 | 2021-03-19 | 远景动力技术(江苏)有限公司 | Non-aqueous electrolyte with high-temperature characteristic and low impedance, application thereof and lithium ion battery |
| CN113161613A (en) * | 2021-04-19 | 2021-07-23 | 杉杉新材料（衢州）有限公司 | Lithium ion battery non-aqueous electrolyte and lithium ion battery |
| CN113161615A (en) * | 2021-06-04 | 2021-07-23 | 湖州昆仑亿恩科电池材料有限公司 | Non-aqueous electrolyte of lithium ion battery and lithium ion battery |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN116344916A (en) * | 2023-05-29 | 2023-06-27 | 宁德时代新能源科技股份有限公司 | Lithium secondary battery and electricity utilization device |
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