CN115000492A - Electrolyte for low-temperature lithium battery - Google Patents
Electrolyte for low-temperature lithium battery Download PDFInfo
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- CN115000492A CN115000492A CN202210718737.1A CN202210718737A CN115000492A CN 115000492 A CN115000492 A CN 115000492A CN 202210718737 A CN202210718737 A CN 202210718737A CN 115000492 A CN115000492 A CN 115000492A
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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
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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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- 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 provides an electrolyte for a low-temperature lithium battery, which comprises the following components: the electrolyte comprises a non-aqueous solvent, electrolyte lithium salt, a borate additive and other additives, wherein the other additives are any one or a mixture of more of Vinylene Carbonate (VC), Biphenyl (BP), triphenyl phosphite (TPP), 1, 3-Propane Sultone (PS), 1, 4-Butane Sultone (BS), Succinic Anhydride (SA) and fluoroethylene carbonate (FEC), and the structural general formula of the borate additive is as follows:
Description
Technical Field
The invention relates to the technical field of lithium battery electrolyte, in particular to electrolyte for a low-temperature lithium battery.
Background
Lithium ion batteries are dominant in the energy storage field today by virtue of their high energy density and high power density in commercial secondary batteries, long cycle life, and the like. Nowadays, the energy density at room temperature of commercial lithium ion batteries has been tripled compared to that of the initial commercialization, but the problem of sudden drop of performance at low temperature is still outstanding, which undoubtedly limits the application of lithium batteries in high-altitude and high-latitude areas, and is also one of the main obstacles for national defense and space applications.
In the lithium ion battery in the prior art, when the external temperature is reduced to-20 ℃ or even lower, the ionic conductivity of the electrolyte can be rapidly reduced, even the electrolyte is frozen, the interface charge transfer kinetics is more slow, the Li + is more difficult to transmit in the SEI and the electrode, and most of the lithium ion batteries based on the Ethylene Carbonate (EC) electrolyte have great energy/power density loss. In addition, lithium plating is likely to occur during low temperature charging, which also presents some safety issues.
Disclosure of Invention
The present invention is directed to solving at least one of the problems of the prior art or the related art.
Therefore, the invention aims to provide the electrolyte for the low-temperature lithium battery, and the borate additive with a special structure is added, so that the viscosity of the electrolyte can be effectively reduced, the ionic conductivity of the lithium battery can be improved, the impedance of the electrolyte under a low-temperature condition can be reduced, and the performance of the lithium battery under the low-temperature condition can be improved.
In order to achieve the above object, an aspect of the present invention provides an electrolyte for a low temperature lithium battery, including: the electrolyte comprises a non-aqueous solvent, electrolyte lithium salt, a borate additive and other additives, wherein the other additives are any one or a mixture of more of Vinylene Carbonate (VC), Biphenyl (BP), triphenyl phosphite (TPP), 1, 3-Propane Sultone (PS), 1, 4-Butane Sultone (BS), Succinic Anhydride (SA) and fluoroethylene carbonate (FEC), and the structural general formula of the borate additive is as follows:
wherein R is 1 ~R 2 Independently of one another, hydrogen, cyano, halo (C1-C10) alk (en) yl, (C1-C10) alk (en) yl, (C1-C10) alkoxy, (C1-C10) alkoxycarbonyl, (C3-C12) cycloalkyl, (C3-C12) heterocycloalkyl, (C6-C12) aryl, (C3-C12) heteroaryl or (C6-C12) aryl (C1-C10) alkyl, pyridine aryl or(unsaturated) aliphatic group.
In the technical scheme, the borate additive with a special structure is added into the electrolyte for the low-temperature lithium battery, so that the viscosity of the electrolyte can be reduced, the conductivity of the electrolyte is improved, a stable interface film is formed on the surface of an electrode more efficiently, the impedance of an SEI film and a CEI film is reduced, and meanwhile, the lithium plating phenomenon in the low-temperature charging process can be effectively relieved by the low-impedance interface film, so that the low-temperature performance of the lithium battery can be improved.
In the above technical solution, preferably, the borate additive is selected from the following structures:
in the technical scheme, the special structure of the borate additive comprises a plurality of B-O bonds, and the boron oxygen heterocycle contains double bonds, so that the viscosity of the electrolyte can be effectively reduced, the conductivity of the electrolyte is improved, a stable interfacial film is efficiently formed on the surface of an electrode, the impedance of the formed interfacial film is low, the lithium plating phenomenon in the low-temperature charging process can be effectively relieved, the compatibility of the borate additive in the electrolyte is good, the conductivity of the electrolyte for the lithium battery under the low-temperature condition can be obviously improved, and the cycle performance and the storage performance of the lithium ion battery under the low-temperature condition can be obviously improved.
In any of the above technical solutions, preferably, the borate additive is dimethyl 3, 4-hydro-1, 2, 5-oxacycloborateThe dosage of the borate additive accounts for 0.01-5% of the total mass of the electrolyte.
In the technical scheme, the electrolyte for the low-temperature lithium battery is further optimized, the 3, 4-hydrogen-1, 2, 5-oxacycloboric acid dimethyl ester is easy to obtain, the compatibility in the electrolyte is better when the dosage is 0.01-5% of the total mass of the electrolyte, the prepared water and acidity can meet the standard, the conductivity is obviously improved under the low-temperature condition (-20 ℃), wherein the conductivity can reach 5.57ms/cm under the low-temperature condition when the dosage of the 3, 4-hydrogen-1, 2, 5-oxacycloboric acid dimethyl ester is 2%, compared with the electrolyte in the prior art, the conductivity is obviously improved, so that the electrolyte has lower impedance under the low-temperature condition and can effectively relieve the lithium plating phenomenon in the low-temperature charging process, the problems of easy discharge and difficult charging of the lithium battery under the low-temperature condition are solved, the thermal stability of the electrolyte is further improved, and the interface side reaction is controlled, so that the safety performance of the battery can be obviously improved.
In any one of the above technical solutions, preferably, the electrolyte lithium salt is any one of lithium hexafluorophosphate (LiPF6), lithium hexafluoroarsenate (LiAsF6), lithium perchlorate (LiClO4), lithium tetrafluoroborate (LiBF4), lithium dioxalate borate (LiBOB) or a mixture of several of them.
In any one of the above technical solutions, preferably, the electrolyte lithium salt is lithium hexafluorophosphate (LiPF6), and the concentration of the electrolyte lithium salt is 1.2 mol/L.
In any one of the above embodiments, preferably, the non-aqueous solvent is any one or a mixture of dimethyl carbonate (DMC), Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC), diethyl carbonate (DEC), Propylene Carbonate (PC) and Methyl Propyl Carbonate (MPC).
In any one of the above technical solutions, preferably, the non-aqueous solvent is a mixture of dimethyl carbonate (DMC), Ethylene Carbonate (EC), and Ethyl Methyl Carbonate (EMC), the amount of the non-aqueous solvent is 60% to 80% of the total mass of the electrolyte, and the mass ratio of dimethyl carbonate (DMC), Ethylene Carbonate (EC), and Ethyl Methyl Carbonate (EMC) is 1:1: 1.
In any of the above technical solutions, preferably, the other additive is a mixture of 1, 4-Butanesultone (BS) and fluoroethylene carbonate (FEC), and the amount of the other additive is 0.01% to 5% of the total mass of the electrolyte.
In any one of the above technical solutions, preferably, the mass fraction of the 1, 4-Butanesultone (BS) is 1.2%, and the mass fraction of the fluoroethylene carbonate (FEC) is 1.2%.
In the technical scheme, the proportion of the electrolyte is further optimized, so that the compatibility of the electrolyte is high, the thermal stability of the electrolyte is further improved, the synergistic effect of the borate additive and other substances can be fully exerted, the viscosity of the electrolyte is further effectively reduced, the conductivity of the electrolyte is improved, the thermal stability of the electrolyte is further improved, the safety performance of the battery is remarkably improved, the low-temperature performance of the battery is improved, the capacity retention rate of the lithium battery can reach 76.48% after the lithium battery is circulated at-20 ℃ for 100 weeks, and the capacity retention rate can reach 84.37% after the lithium battery is stored at-20 ℃ for 7 days.
The technical scheme of the invention also provides a low-temperature lithium battery, and the electrolyte for the low-temperature lithium battery in the technical scheme is adopted, so that all beneficial technical effects of the electrolyte for the low-temperature lithium battery in the technical scheme are achieved, and the details are not repeated herein.
The electrolyte for the low-temperature lithium battery provided by the invention has the following beneficial technical effects:
(1) the borate additive with a special structure is added into the electrolyte for the low-temperature lithium battery, so that the viscosity of the electrolyte can be effectively reduced, the ionic conductivity of the lithium battery can be improved, the electrolyte has lower impedance under a low-temperature condition, and the borate additive has good compatibility in the electrolyte and can be cooperated with other substances in the electrolyte to effectively improve the low-temperature performance of the electrolyte.
(2) The borate additive with a special structure is added into the electrolyte for the low-temperature lithium battery, the borate additive comprises a plurality of B-O bonds, and double bonds are contained in boron-oxygen heterocycles, so that a stable interface film can be formed on the surface of an electrode more efficiently, and the impedances of SEI and CEI are reduced, so that the low-temperature performance of the lithium battery is improved, the capacity retention rate of the lithium battery can reach 76.48% after the lithium battery is cycled at-20 ℃ for 100 weeks, and the capacity retention rate of the lithium battery can reach 84.37% after the lithium battery is stored at-20 ℃ for 7 days. Meanwhile, the low-impedance interface film is beneficial to relieving the lithium plating phenomenon in the low-temperature charging process, and the problems of easiness in discharging and difficulty in charging of the lithium battery under the low-temperature condition are effectively solved.
(3) The borate additive with a special structure is added into the electrolyte for the low-temperature lithium battery, and the B-O bond contained in the borate additive can improve the electrochemical and thermodynamic stability of the lithium battery, control the interface side reaction and further improve the safety performance of the lithium battery.
Additional aspects and advantages of the invention will be set forth in part in the description which follows, and in part will be obvious from the description, or may be learned by practice of the invention.
Detailed Description
The invention discloses an electrolyte for a low-temperature lithium battery, which can be realized by appropriately improving process parameters by referring to the contents in the field. It is expressly intended that all such similar substitutes and modifications which would be obvious to one skilled in the art are deemed to be included in the invention. While the methods and applications of this invention have been described in terms of preferred embodiments, it will be apparent to those of skill in the art that variations and modifications, or appropriate variations and combinations of the methods and applications described herein may be made to implement and use the techniques of this invention without departing from the spirit and scope of the invention.
The invention is further illustrated by the following examples:
example 1
Under the airtight protection atmosphere of nitrogen, under the condition that the moisture content is less than 10ppm, sequentially adding and mixing non-aqueous solvents of Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC) and diethyl carbonate (DEC) according to the mass ratio of 1:1:1, cooling the mixed solution by using a condenser to ensure that the temperature is not higher than 10 ℃, slowly adding lithium hexafluorophosphate to ensure that the concentration of lithium salt is 1.2mol/L, then adding 1, 4-Butyl Sultone (BS) with the mass fraction of 1.2% and 1.2% fluoroethylene carbonate (FEC), adding 3, 4-hydro-1, 2, 5-oxacycloboric acid dimethyl ester with the mass fraction of 0.5%, and continuously stirring until the solution becomes clear.
Example 2
The difference from example 1 is that 1% by weight of dimethyl 3, 4-hydro-1, 2, 5-oxacycloborate is added and stirring is continued until the solution becomes clear.
Example 3
The difference from example 1 is that 1.5% by weight of dimethyl 3, 4-hydro-1, 2, 5-oxocycloborate is added and stirring is continued until the solution becomes clear.
Example 4
The difference from example 1 is that 2% by weight of dimethyl 3, 4-hydro-1, 2, 5-oxacycloborate is added and stirring is continued until the solution becomes clear.
Example 5
The difference from example 1 is that 2.5% by weight of dimethyl 3, 4-hydro-1, 2, 5-oxacycloborate is added and stirring is continued until the solution becomes clear.
Example 6
The difference from example 1 is that 3% by weight of dimethyl 3, 4-hydro-1, 2, 5-oxacycloborate is added and stirring is continued until the solution becomes clear.
Comparative example 1
Under the nitrogen sealed protection atmosphere, under the condition that the moisture content is less than 10ppm, sequentially adding and mixing non-aqueous solvents of Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC) and diethyl carbonate (DEC) according to the mass ratio of 1:1:1, cooling the mixed solution by using a condenser to ensure that the temperature is not higher than 10 ℃, slowly adding lithium hexafluorophosphate to ensure that the concentration of lithium salt is 1.2mol/L, and then adding 1, 4-Butyl Sultone (BS) with the mass fraction of 1.2% and 1.2% fluoroethylene carbonate (FEC) and stirring until the solution becomes clear.
Comparative example 2
Under the airtight protection atmosphere of nitrogen, under the condition that the moisture content is less than 10ppm, sequentially adding and mixing non-aqueous solvents of Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC) and diethyl carbonate (DEC) according to the mass ratio of 1:1:1, cooling the mixed solution by using a condenser to ensure that the temperature is not higher than 10 ℃, slowly adding lithium hexafluorophosphate to ensure that the concentration of lithium salt is 1.2mol/L, then adding 1, 4-Butyl Sultone (BS) with the mass fraction of 1.2% and 1.2% fluoroethylene carbonate (FEC), adding 3% dimethyl borate with the mass fraction, and continuously stirring until the solution becomes clear.
The electrolytes prepared in the above examples 1 to 6 and comparative examples 1 and 2 were tested for moisture, acidity and conductivity, and the test results are shown in table 1 below.
Table 1 moisture, acidity and conductivity test results for electrolytes
As can be seen from table 1, the electrolytes prepared in examples 1 to 6 and comparative examples 1 and 2 have acceptable values of medium moisture and acidity, and when the electrolyte conductivity is increased to a certain value at a low temperature (-20 ℃), the electrolyte conductivity is increased with the increase of the borate additive, but when the electrolyte conductivity is increased to a certain value, the electrolyte conductivity is decreased, and when the mass fraction of the borate additive is 2%, the effect is good, and the conductivity can reach 5.57ms/cm at a low temperature. Compared with the example 6, the specific structure of the dimethyl 3, 4-hydrogen-1, 2, 5-oxacycloborate can more efficiently form a stable interfacial film on the surface of an electrode, reduce the resistance of SEI and CEI, and further improve the low-temperature performance of the lithium battery. Compared with the traditional dimethyl borate, the 3, 4-hydrogen-1, 2, 5-oxacycloborate dimethyl ester obviously improves the conductivity, and can obtain higher conductivity with the dosage of 2 percent, less dosage and high compatibility in electrolyte.
Lithium ion batteries were prepared using the electrolytes formulated in examples 1 to 6 and comparative examples 1 and 2 described above.
The anode and the cathode respectively adopt ternary materials LiNi8Co1Mn1O2, Super-P, PVDF (900, 5130) and CNT; uniformly mixing a silicon carbon material (450mAh/g), Super-P, CMC, SBR and the like according to a certain proportion to prepare positive and negative electrode slurry with certain viscosity, then respectively and uniformly coating the positive and negative electrode slurry on aluminum and copper current collectors, drying at 80 ℃, then finishing the manufacture of a battery cell through the working procedures of cutting, rolling, slitting, winding into a shell and the like, finally drying at 85 ℃ for 48 hours, injecting the electrolyte, and finishing the manufacture of a lithium ion battery after packaging. The lithium ion battery is subjected to hot pressing formation and vacuum secondary sealing, and then subjected to low-temperature cycle test at 0 +/-20 ℃ and storage test at 0 +/-20 ℃. The test results are shown in table 2 below.
TABLE 2 Low temperature cycling test at 0 ℃/-20 ℃ and storage test results at 0 ℃/-20 ℃ for lithium batteries
As shown in Table 2, the use of the borate additive obviously improves the cycle performance of the lithium ion battery under low temperature conditions, and is beneficial to improving the storage performance of the lithium ion battery under low temperature conditions, improving the thermal stability of the electrolyte, controlling the interface side reaction and improving the safety performance of the battery. Wherein, when the mass fraction of the dimethyl 3, 4-hydro-1, 2, 5-oxacycloborate in the embodiment 5 is 2%, the effect is better, the capacity retention rate of the lithium battery can reach 76.48% after the lithium battery is cycled at-20 ℃ for 100 weeks, and the capacity retention rate can reach 84.37% after the lithium battery is stored at-20 ℃ for 7 days. Moreover, compared with the traditional dimethyl borate, the addition of 3, 4-hydrogen-1, 2, 5-oxacyclodimethyl borate obviously improves the capacity retention rate of 100 weeks in a circulation at the temperature of-20 ℃ and the capacity retention rate of 7 days in storage. The addition of the borate additive with a special structure can more efficiently form a stable interface film on the surface of the electrode, so that the conductivity of the lithium ion battery under a low-temperature condition is improved, the electrolyte has lower impedance under the low-temperature condition, and meanwhile, the stable interface film is formed on the surface of the electrode, so that the low-temperature performance of the lithium ion battery is improved. In addition, the B-O bond contained in the borate additive can improve the electrochemical and thermodynamic stability of the lithium battery, thereby improving the safety performance of the lithium battery.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and amendments can be made without departing from the principle of the present invention, and these modifications and amendments should also be considered as the protection scope of the present invention.
Claims (10)
1. An electrolyte for a low-temperature lithium battery, comprising: the electrolyte comprises a non-aqueous solvent, electrolyte lithium salt, a borate additive and other additives, wherein the other additives are any one or a mixture of more of Vinylene Carbonate (VC), Biphenyl (BP), triphenyl phosphite (TPP), 1, 3-Propane Sultone (PS), 1, 4-Butane Sultone (BS), Succinic Anhydride (SA) and fluoroethylene carbonate (FEC), and the structural general formula of the borate additive is as follows:
wherein R is 1 ~R 2 Independently of one another, hydrogen, cyano, halo (C1-C10) alk (en) yl, (C1-C10) alk (en) yl, (C1-C10) alkoxy, (C1-C10) alkoxycarbonyl, (C3-C12) cycloalkyl, (C3-C12) heterocycloalkyl, (C6-C12) aryl, (C3-C12) heteroaryl or (C6-C12) aryl (C1-C10) alkyl, pyridine aromatic or (unsaturated) aliphatic.
4. The electrolyte for a low-temperature lithium battery according to any one of claims 1 to 3,
the electrolyte lithium salt is any one of lithium hexafluorophosphate (LiPF6), lithium hexafluoroarsenate (LiAsF6), lithium perchlorate (LiClO4), lithium tetrafluoroborate (LiBF4) and lithium dioxalate borate (LiBOB) or a mixture of a plurality of the lithium hexafluorophosphate, the lithium hexafluoroarsenate (LiAsF6), the lithium perchlorate (LiClO4), the lithium tetrafluoroborate and the lithium dioxalate borate (LiBOB).
5. The electrolyte for a low-temperature lithium battery according to claim 4,
the electrolyte lithium salt is lithium hexafluorophosphate (LiPF6), and the concentration of the electrolyte lithium salt is 1.2 mol/L.
6. The electrolyte for a low-temperature lithium battery according to claim 1, wherein the non-aqueous solvent is any one or a mixture of dimethyl carbonate (DMC), Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC), diethyl carbonate (DEC), Propylene Carbonate (PC) and Methyl Propyl Carbonate (MPC).
7. The electrolyte for a low-temperature lithium battery according to claim 6, wherein the non-aqueous solvent is a mixture of dimethyl carbonate (DMC), Ethylene Carbonate (EC) and Ethyl Methyl Carbonate (EMC), the amount of the non-aqueous solvent is 60-80% of the total mass of the electrolyte, and the mass ratio of the dimethyl carbonate (DMC), the Ethylene Carbonate (EC) and the Ethyl Methyl Carbonate (EMC) is 1:1: 1.
8. The electrolyte for a low-temperature lithium battery according to claim 1,
the other additive is a mixture of 1, 4-Butyl Sultone (BS) and fluoroethylene carbonate (FEC), and the using amount of the other additive is 0.01-5% of the total mass of the electrolyte.
9. The electrolyte for a low-temperature lithium battery according to claim 8,
the mass fraction of the 1, 4-Butanesultone (BS) is 1.2%, and the mass fraction of the fluoroethylene carbonate (FEC) is 1.2%.
10. A low-temperature lithium battery, characterized in that the electrolyte for a low-temperature lithium battery as claimed in any one of claims 1 to 9 is used.
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