CN112038697A - Lithium ion battery non-aqueous electrolyte and lithium ion battery - Google Patents
Lithium ion battery non-aqueous electrolyte and lithium ion battery Download PDFInfo
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- CN112038697A CN112038697A CN202010885898.0A CN202010885898A CN112038697A CN 112038697 A CN112038697 A CN 112038697A CN 202010885898 A CN202010885898 A CN 202010885898A CN 112038697 A CN112038697 A CN 112038697A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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Abstract
The invention provides a lithium ion battery non-aqueous electrolyte and a lithium ion battery, wherein the lithium ion battery non-aqueous electrolyte comprises a solvent, a lithium salt and an additive, and the additive comprises a compound shown in a structural formula (1). According to the invention, the compound with the structure (1) is introduced as an electrolyte additive, so that the circulation and high-temperature performance of the electrolyte can be effectively improved, and the service life of the lithium battery is prolonged.
Description
Technical Field
The invention belongs to the field of lithium ion batteries, and relates to a lithium ion battery non-aqueous electrolyte and a lithium ion battery.
Background
In recent years, under the double promotion of market and policy, the new energy industry is rapidly developed. Compared with the traditional secondary charging technology, the lithium ion battery has the obvious advantages of high energy density, long cycle life, environmental protection, no pollution and the like, and has an absolutely leading effect in the fields of power automobiles, energy storage, digital products and the like. However, with the popularization of lithium ion battery technology in various living fields, people have not met the existing performance, and especially have made higher requirements on the service life and the service temperature of the lithium ion battery.
The electrolyte is one of four main materials of a lithium battery and mainly comprises three components of lithium salt, a solvent and an additive. The difference of the three components directly determines the performance of the electrolyte, and further influences the performance of the lithium ion battery. The additive has the characteristics of small dosage, quick response and the like, and can well improve the performance of the lithium ion battery, so that the development of a novel additive and related electrolyte becomes an effective way for improving the performance of the lithium ion battery.
Disclosure of Invention
In view of the defects of the prior art, the invention aims to provide a lithium ion battery nonaqueous electrolyte and a lithium ion battery. The non-aqueous electrolyte of the lithium ion battery can improve the performance of the lithium ion battery and prolong the service life of the lithium ion battery.
In order to achieve the purpose, the invention adopts the following technical scheme:
in one aspect, the present invention provides a lithium ion battery nonaqueous electrolyte, including a solvent, a lithium salt, and an additive, where the additive includes a compound represented by structural formula (1):
wherein, the R group is any one of alkyl of C1-C4 (such as C1, C2, C3 or C4), perfluorinated or partially fluorinated alkyl of C1-C4, halogen atom or cyano.
In the invention, the compound of the structural formula (1) is a phosphate compound, which can improve the high-temperature performance of the formed SEI film, then the double bond structure can carry out ring-opening reaction in the electrochemical process to form the SEI film, which can well protect the anode and the cathode, and the five-membered ring structure can carry out ring-opening reaction to absorb oxygen, hydrofluoric acid and the like generated after long circulation to a certain extent, and finally, the matching of lithium salt, solvent and additive can further achieve the effects of improving the performance and prolonging the service life.
Preferably, the compound represented by the structural formula (1) is one or a combination of at least two selected from the following compounds a to D:
Preferably, the amount of the compound represented by the structural formula (1) is 0.001% to 8%, for example, 0.001%, 0.005%, 0.008%, 0.01%, 0.05%, 0.08%, 0.1%, 0.5%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, or 8% based on 100% by mass of the total of the nonaqueous electrolyte solution for a lithium ion battery.
Preferably, the solvent is any one of carbonate, carboxylate and phosphate solvents or a combination of at least two thereof.
Preferably, the carbonate-based solvent is selected from one or a combination of at least two of dimethyl carbonate (DMC), diethyl carbonate (DEC), Ethyl Methyl Carbonate (EMC), dipropyl carbonate (DPC), ethyl propyl carbonate, dibutyl carbonate, Ethylene Carbonate (EC), Propylene Carbonate (PC).
Preferably, the carboxylic ester solvent is selected from one or a combination of at least two of ethyl valerate, propyl valerate, butyl valerate, Ethyl Butyrate (EB), propyl butyrate, butyl butyrate, Ethyl Propionate (EP), Propyl Propionate (PP), butyl propionate, methyl acetate, Ethyl Acetate (EA), propyl acetate, butyl acetate.
Preferably, the phosphate-based solvent is selected from one or a combination of at least two of trimethyl phosphate, triethyl phosphate, tris (2-chloroethyl) phosphate, tris (2,2, 2-trifluoroethyl) phosphate, tripropyl phosphate, triisopropyl phosphate, tributyl phosphate, trihexyl phosphate, triphenyl phosphate, tricresyl phosphate, methylethylene phosphate or ethylethylene phosphate.
Preferably, the carbonate-based solvent is contained in an amount of 20 to 85% by mass, for example, 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80% or 85% by mass based on 100% by mass of the total nonaqueous electrolyte solution for a lithium ion battery.
Preferably, the content of the carboxylic ester solvent is 0 to 35% by mass, for example, 0.5%, 0.8%, 1%, 3%, 5%, 8%, 10%, 15%, 18%, 20%, 25%, 28%, 30% or 35% by mass, based on 100% by mass of the total mass of the lithium ion battery nonaqueous electrolyte solution.
Preferably, the phosphate-based solvent is contained in an amount of 0 to 20% by mass, for example, 0.5%, 0.8%, 1%, 3%, 5%, 8%, 10%, 15%, 18%, 20% by mass, based on 100% by mass of the total nonaqueous electrolyte solution for a lithium ion battery.
Preferably, the lithium salt is selected from lithium hexafluorophosphate (LiPF)6) Lithium hexafluoroarsenate (LiAsF)6) Lithium difluorophosphate (LiPO)2F2) Lithium tetrafluoroborate (LiBF)4) Lithium perchlorate (LiClO)4) One or a combination of at least two of lithium bis fluorosulfonylimide (LiFSI) or lithium bis trifluoromethanesulfonylimide (LiTFSI).
Preferably, the lithium salt is present in an amount of 3 to 18% by mass, for example 3%, 5%, 7%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17% or 18% by mass, based on 100% by mass of the total nonaqueous electrolyte solution of the lithium ion battery.
Preferably, the additive further includes other additives than the compound represented by structural formula (1).
Preferably, the other additive is one or a combination of at least two of Vinylene Carbonate (VC), ethylene carbonate (abbreviated as VEC), 1, 3-Propane Sultone (PS), 1, 4-Butane Sultone (BS), or vinyl sulfate (DTD).
Preferably, the content of the other additive is 0.01% to 5%, for example, 0.01%, 0.05%, 0.08%, 0.1%, 0.5%, 0.8%, 1%, 2%, 3%, 4%, or 5%, based on 100% by mass of the total nonaqueous electrolyte solution of the lithium ion battery.
In a second aspect, the present invention provides a lithium ion battery comprising a positive electrode, a negative electrode, a separator disposed between the positive electrode and the negative electrode, and an electrolyte, wherein the electrolyte is the lithium ion battery non-aqueous electrolyte as described above.
In the present invention, the positive electrode, the negative electrode, and the separator are not particularly limited, and any of the positive electrode, the negative electrode, and the separator that are conventional in the art can be used.
The lithium ion battery non-aqueous electrolyte provided by the invention effectively improves the cycle and high-temperature storage performance of the battery, and the lithium ion battery containing the non-aqueous electrolyte has excellent cycle performance and high-temperature storage performance and prolongs the service life.
Compared with the prior art, the invention has the following beneficial effects:
according to the invention, the compound of the structural formula (1) is used as an electrolyte additive, so that the high-temperature performance of the formed SEI film can be improved, the structure of the double bond can perform ring-opening reaction in the electrochemical process to form the SEI film, the anode and the cathode can be well protected, the structure of the five-membered ring can perform ring-opening reaction to absorb oxygen, hydrofluoric acid and the like generated after long circulation, the cycle performance and the high-temperature resistance of the lithium ion battery are improved, and the service life is prolonged.
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.
Comparative example 1
In a dry argon atmosphere glove box (moisture)<1ppm, oxygen gas<1ppm), Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC), diethyl carbonate (DEC) were mixed according to EC: EMC: DEC ═ 3:mixing at a ratio of 5:2, adding 1M LiPF after mixing uniformly6And then fully stirring, and obtaining the required electrolyte after fully dissolving.
Comparative example 2
An electrolyte was prepared according to the method of comparative example 1, except that Vinylene Carbonate (VC) was added in an amount of 1% by weight.
Example 1
An electrolyte was prepared according to the method of comparative example 1, except that compound a was added in an amount of 1% by weight.
Example 2
An electrolyte was prepared according to the method of comparative example 1, except that Vinylene Carbonate (VC) and compound a were added in the amounts of 1% and 0.5%, respectively.
Example 3
An electrolyte was prepared according to the method of comparative example 1, except that Vinylene Carbonate (VC) and compound a were added in the amounts of 1% and 1%, respectively.
Example 4
An electrolyte was prepared according to the method of comparative example 1, except that Vinylene Carbonate (VC) and compound a were added in the amounts of 1% and 1.5%, respectively.
Example 5
An electrolyte was prepared according to the method of comparative example 1, except that Vinylene Carbonate (VC) and compound B were added in the amounts of 1% and 1%, respectively.
Example 6
An electrolyte was prepared according to the method of comparative example 1, except that Vinylene Carbonate (VC) and compound C were added in the amounts of 1% and 1%, respectively.
Comparative example 3
An electrolyte was prepared according to the method of comparative example 1, except that lithium difluorophosphate (LiPO) was added2F2) Vinylene Carbonate (VC) and vinyl sulfate (DTD), in percentages of 0.5%, 1% and 0.5%, respectively.
Example 7
An electrolyte was prepared according to the method of comparative example 2, except that compound a was added in an amount of 0.5% by weight.
Example 8
An electrolyte was prepared according to the method of comparative example 2, except that compound a was added in an amount of 1% by weight.
Example 9
An electrolyte was prepared according to the method of comparative example 2, except that the compound B was added in an amount of 0.5% by weight.
Example 10
An electrolyte was prepared according to the method of comparative example 2, except that compound B was added in an amount of 1% by weight.
Comparative example 4
An electrolyte was prepared according to the method of comparative example 1, except that lithium bis-fluorosulfonylimide (LiFSI), Vinylene Carbonate (VC), and vinyl sulfate (VEC) were added in the amounts of 0.5%, 1%, and 0.3%, respectively.
Example 11
An electrolyte was prepared according to the method of comparative example 3, except that compound C was added in an amount of 0.5% by weight.
Example 12
An electrolyte was prepared according to the method of comparative example 3, except that compound C was added in an amount of 1% by weight.
Example 13
An electrolyte was prepared according to the method of comparative example 3, except that compound C was added in an amount of 3%.
Example 14
An electrolyte was prepared according to the method of comparative example 3, except that compound C was added in an amount of 5%.
Example 15
An electrolyte was prepared according to the method of comparative example 3, except that compound C was added in an amount of 7% by weight.
Comparative example 5
An electrolyte was prepared according to the method of comparative example 3, except that compound C was added in an amount of 9% by weight.
The electrolyte formulations of comparative examples 2 to 5 and examples 1 to 15 are shown in table 1 (wherein the contents of the respective components are contents based on the total mass of the electrolyte as 100).
TABLE 1
The secondary lithium batteries of examples 1 to 15 and comparative examples 1 to 5 were fabricated as follows.
(1) Preparing a positive plate: LiNi-Co-Mn ternary material0.5Co0.2Mn0.3O2Mixing polyvinylidene fluoride serving as a binder and acetylene black serving as a conductive agent according to a mass ratio of 90:5:5, adding N-methyl pyrrolidone (NMP), mixing and stirring uniformly to obtain anode slurry; uniformly coating the positive electrode slurry on a positive electrode current collector aluminum foil with the thickness of 14 mu m; and drying the aluminum foil at room temperature, then carrying out cold pressing and slitting to obtain the positive plate.
(2) Preparing a negative plate: mixing the cathode active material mesocarbon microbeads (MCMB), carbon black and a binder polyvinylidene fluoride according to a mass ratio of 88:5:7, adding N-methylpyrrolidone (NMP), mixing and stirring uniformly to obtain cathode slurry; uniformly coating the negative electrode slurry on a negative electrode current collector copper foil with the thickness of 10 mu m; and drying the copper foil at room temperature, then carrying out cold pressing and slitting to obtain the negative plate.
(3) Preparing an isolating membrane: the double-sided ceramic-coated polyethylene is used as a separation film, the thickness of the polyethylene-based film is 12 μm, and the thickness of the coating layer is 3 μm.
(4) Preparing a lithium ion battery: and (3) stacking the positive plate, the isolating film and the negative plate in a lamination mode, then loading the positive plate, the isolating film and the negative plate into an aluminum-plastic film, drying (the water content of the plates is less than 100ppm), then injecting corresponding electrolyte and sealing, and carrying out the procedures of standing, formation, final sealing, capacity grading and the like to obtain the lithium ion battery.
(5) The nominal capacity of the cell design is 5 Ah.
The secondary lithium batteries of examples 1 to 12 and comparative examples 1 to 3 were subjected to cycle testing in the following manner:
the cell was left to stand in a constant temperature oven at 45 ℃ for 24 hours, and then subjected to cycle performance test. The cycle voltage was 3.0-4.3V, the current was 1C (5A), and the time between charging and discharging was 10 minutes.
Capacity retention (%) — N-th week discharge capacity/1-th week discharge capacity.
The lithium secondary batteries of examples 1 to 12 and comparative examples 1 to 3 were subjected to a high-temperature storage test in the following manner:
at normal temperature, the battery is charged and discharged for 3 times by using the current of 1C (5A), the voltage range is 3-4.3V, the third discharge capacity is taken as the initial discharge capacity, then the battery is charged to full charge voltage according to the cell of 1C, then the battery is placed in an oven at 70 ℃ for storage for seven days, then the battery is placed at room temperature for full cooling, and finally the capacity retention rate and the recovery rate are tested.
The 45 ℃ cycle performance and 70 ℃ high temperature storage performance of the electrolyte formulations of comparative examples 1-5 and examples 1-15 are shown in table 2.
TABLE 2
Comparing example 1 with comparative examples 1 and 2, it can be seen that compound a has a certain film-forming effect, the double bond structure of which can react during formation, and can exert an effective film-forming effect even in an electrolyte without an additive, thereby stabilizing the battery structure and prolonging the battery life.
Comparing example 2 with comparative example 2, it can be found that the compound a added to the electrolyte can be well matched with VC, and the cycle performance and storage performance of the lithium battery can be improved.
Comparing examples 2, 3, 4 with comparative example 2, it can be seen that the cycling performance at 1% level is higher than the cycling performance at 0.5% level and 1.5% level when compound a is used in combination with VC, indicating that compound a is not used as much as possible at higher levels and needs to be used within a reasonable range.
Comparing comparative example 2 with examples 7 and 9, and comparative example 3 with example 11, it can be seen that the introduction of compounds A, B and C can both improve the cycle performance and high temperature performance of the lithium ion battery very well, and in particular can still function in multi-additive electrolytes.
The results show that the compound of the structural formula (1) can form a good SEI film on the surfaces of the positive electrode and the negative electrode of the lithium battery to protect the positive electrode and the negative electrode, and the electrolyte formed by combining the compound with different lithium salts, solvents and additives can effectively prolong the service life of the lithium battery and simultaneously improve the high-temperature resistance of the lithium battery.
The applicant states that the present invention is described by the above examples of the lithium ion battery nonaqueous electrolytic solution and the lithium ion battery of the present invention, but the present invention is not limited to the above examples, that is, the present invention is not limited to the above examples. It should be understood by those skilled in the art that any modification of the present invention, equivalent substitutions of the raw materials of the product of the present invention, addition of auxiliary components, selection of specific modes, etc., are within the scope and disclosure of the present invention.
Claims (10)
1. The non-aqueous electrolyte for the lithium ion battery is characterized by comprising a solvent, a lithium salt and an additive, wherein the additive comprises a compound shown in a structural formula (1):
wherein, the R group is any one of C1-C4 alkyl, perfluorinated or partially fluorinated C1-C4 alkyl, halogen atom or cyano.
2. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the compound represented by the structural formula (1) is one or a combination of at least two selected from the following compounds a to D:
3. the nonaqueous electrolyte solution for lithium ion batteries according to claim 1 or 2, wherein the amount of the compound represented by the structural formula (1) is 0.001% to 8% based on 100% by mass of the total amount of the nonaqueous electrolyte solution for lithium ion batteries.
4. The nonaqueous electrolyte solution for a lithium ion battery according to any one of claims 1 to 3, wherein the solvent is any one of carbonate, carboxylate and phosphate solvents or a combination of at least two thereof.
5. The nonaqueous electrolyte solution for lithium ion batteries according to claim 4, wherein the carbonate-based solvent is selected from one or a combination of at least two of dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, dipropyl carbonate, ethyl propyl carbonate, dibutyl carbonate, ethylene carbonate, and propylene carbonate;
preferably, the carboxylic ester solvent is selected from one or a combination of at least two of ethyl valerate, propyl valerate, butyl valerate, ethyl butyrate, propyl butyrate, butyl butyrate, ethyl propionate, propyl propionate, butyl propionate, methyl acetate, ethyl acetate, propyl acetate and butyl acetate;
preferably, the phosphate-based solvent is selected from one or a combination of at least two of trimethyl phosphate, triethyl phosphate, tris (2-chloroethyl) phosphate, tris (2,2, 2-trifluoroethyl) phosphate, tripropyl phosphate, triisopropyl phosphate, tributyl phosphate, trihexyl phosphate, triphenyl phosphate, tricresyl phosphate, methylethylene phosphate or ethylethylene phosphate.
6. The nonaqueous electrolyte solution for lithium ion batteries according to claim 4, wherein the carbonate-based solvent is contained in an amount of 20 to 85% by mass based on 100% by mass of the total mass of the nonaqueous electrolyte solution for lithium ion batteries;
preferably, the mass percentage of the carboxylic ester solvent is 0-35% based on 100% of the total mass of the non-aqueous electrolyte of the lithium ion battery;
preferably, the phosphate ester solvent is 0-20% by mass based on 100% by mass of the total mass of the lithium ion battery nonaqueous electrolyte.
7. The nonaqueous electrolyte solution for a lithium ion battery according to any one of claims 1 to 6, wherein the lithium salt is selected from one or a combination of at least two of lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium difluorophosphate, lithium tetrafluoroborate, lithium perchlorate, lithium bis (fluorosulfonyl) imide and lithium bis (trifluoromethanesulfonyl) imide;
preferably, the lithium salt accounts for 3-18% of the total mass of the lithium ion battery nonaqueous electrolyte solution as 100%.
8. The nonaqueous electrolyte solution for a lithium ion battery according to any one of claims 1 to 7, wherein the additive further comprises an additive other than the compound represented by the structural formula (1);
preferably, the other additive is one or a combination of at least two of vinylene carbonate, ethylene carbonate, 1, 3-propane sultone, 1, 4-butane sultone or vinyl sulfate.
9. The nonaqueous electrolyte solution for lithium ion batteries according to any one of claims 1 to 8, wherein the content of the other additive is 0.01 to 5% based on 100% by mass of the total mass of the nonaqueous electrolyte solution for lithium ion batteries.
10. A lithium ion battery comprising a positive electrode, a negative electrode, a separator provided between the positive electrode and the negative electrode, and an electrolytic solution, wherein the electrolytic solution is the lithium ion battery nonaqueous electrolytic solution according to any one of claims 1 to 9.
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