CN111129595A - High-voltage lithium ion battery non-aqueous electrolyte and lithium ion battery containing electrolyte - Google Patents
High-voltage lithium ion battery non-aqueous electrolyte and lithium ion battery containing electrolyte Download PDFInfo
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- CN111129595A CN111129595A CN201911364517.8A CN201911364517A CN111129595A CN 111129595 A CN111129595 A CN 111129595A CN 201911364517 A CN201911364517 A CN 201911364517A CN 111129595 A CN111129595 A CN 111129595A
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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
Abstract
The invention discloses a high-voltage lithium ion battery non-aqueous electrolyte, which comprises a non-aqueous organic solvent, an electrolyte and an additive, wherein the additive comprises the following components in percentage by mass in the lithium ion battery non-aqueous electrolyte: 0.1-5% of silane isocyanate additive and 0.1-5% of low-impedance additive. The invention also discloses a lithium ion battery comprising the anode, the cathode, the diaphragm and the high-voltage lithium ion battery non-aqueous electrolyte. The high-voltage lithium ion battery non-aqueous electrolyte can improve the electrochemical performance of the lithium ion battery through the synergistic effect of the components, particularly reduce the impedance and generate gas at high temperature, and greatly improve the cycle life.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to a high-voltage lithium ion battery non-aqueous electrolyte and a lithium ion battery containing the same.
Background
Over the past decade, the need for more energy dense, longer cycle and calendar life, reinforced energy storage systems based on low cost materials and processes has increased dramatically. The advent of electric vehicles in particularAnd market growth, as well as the success of portable consumer electronics, have led to interest in high energy density LIBs. The energy (E) of the battery is determined by the product of the average voltage (U) and the charge (Q) of the battery. Since the redox potential of the negative electrode material graphite in lithium ion batteries is already very close to that of metallic lithium, the battery voltage can only be increased by higher cathode potentials. However, conventional electrolytes employ an organic carbonate solvent, such as Ethylene Carbonate (EC) and Ethyl Methyl Carbonate (EMC), to dissolve LiPF6The normal working voltage of the mixed solution is below 4.2V (vs. Li/Li +), and continuous decomposition is continuously carried out when the voltage exceeds 4.4V (vs. Li/Li +). In addition, parasitic reactions occur between the cathode surface and the electrolyte, resulting in surface reconstruction of the cathode material. Therefore, maintaining a stable interface is critical to improving the electrochemical performance of the cathode material at high pressure. At present, the formation of an inert protective layer on the surface of a material by adding a film-forming additive is an effective way to improve the interface stability.
For example, chinese patent CN105990605A discloses a nonaqueous electrolytic solution comprising a lithium salt, a nonaqueous solvent and an additive containing trimethylsilyl isocyanate and orthoester. The invention also provides a lithium ion battery adopting the non-aqueous electrolyte. In the non-aqueous electrolyte provided by the invention, the high-temperature performance of the battery can be effectively improved by adopting the trimethylsilyl isocyanate and the orthocarbonate as specific additives. The disadvantage is that the cycle life of the battery is still not ideal.
Disclosure of Invention
In view of the problems of the prior art, the invention aims to provide a high-voltage lithium ion battery non-aqueous electrolyte and a lithium ion battery containing the electrolyte. The high-voltage lithium ion battery non-aqueous electrolyte can improve the electrochemical performance of the lithium ion battery through the synergistic effect of all the components, particularly reduce the impedance and generate gas at high temperature, and greatly improve the cycle life.
In order to achieve the purpose, the invention adopts the technical scheme that: the non-aqueous electrolyte of the high-voltage lithium ion battery comprises a non-aqueous organic solvent, an electrolyte and an additive, wherein the additive comprises the following components in percentage by mass in the non-aqueous electrolyte of the lithium ion battery:
silane isocyanate additive 0.1-5%
Low impedance additive 0.1-5%
As a preferred embodiment of the present invention, the silane based isocyanate based additive has the following formula:
wherein R is1,R2,R3,R4Each independently selected from a substituted or unsubstituted alkyl group having 1 to 10 carbon atoms, an alkenyl group having 2 to 10 carbon atoms, and an aralkyl group having 6 to 10 carbon atoms.
As a preferred embodiment of the present invention, the silane based isocyanate based additive is selected from at least one of the compounds represented by the following structural formula:
as a preferred embodiment of the invention, the low impedance additive is selected from the group consisting of Vinylene Carbonate (VC), 1, 3-Propanesultone (PS), vinyl sulfate (DTD), tris (trimethylsilane) borate (TMSB), tris (trimethylsilane) phosphate (TMSP), lithium difluorophosphate (LiDFP), lithium difluorooxalato borate (LiDFOB), lithium bis (LiBOB) oxalato borate (LiBOB), lithium tetrafluoroborate (LiBF)4) At least one of lithium bis (sulfonamide) imide (LiFSI) and lithium bis (trifluoromethyl) sulfonyl imide (LiTFSI).
As a preferred embodiment of the present invention, the non-aqueous organic solvent is at least one selected from the group consisting of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, ethyl methyl carbonate, propyl ethyl carbonate, ethyl acetate, ethyl propionate, ethyl butyrate, propyl acetate, propyl propionate, butyl butyrate, fluoroethylene carbonate, ethylene difluorocarbonate, ethyl fluoroformate, ethyl fluoroacetate, propyl fluoroformate, propyl fluoropropionate, butyl fluoroformate, butyl fluoroacetate, dimethyl sulfone, sulfolane, and 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether. The non-aqueous organic solvent is more preferably at least three of Ethylene Carbonate (EC), fluoroethylene carbonate (FEC), 1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether (D2), fluoroethylene carbonate (FEMC), difluoroethylene carbonate (HFDEC), and Ethyl Propionate (EP).
The electrolyte in the present invention is not limited as long as it is used as an electrolyte in a nonaqueous electrolyte secondary battery, and a known electrolyte may be used arbitrarily. When the high-voltage lithium ion battery nonaqueous electrolyte of the present invention is used for a lithium secondary battery, a lithium salt is generally used as an electrolyte, and as a preferred embodiment of the present invention, the electrolyte is at least one of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium difluorophosphate, lithium bis (oxalato) borate, lithium difluorooxalato borate, lithium tetrafluorooxalato phosphate, lithium difluorooxalato phosphate, lithium bis (fluorosulfonyl) imide, lithium bis (trifluoromethanesulfonyl) imide, and lithium fluorosulfonyl (trifluoromethanesulfonyl methyl) imide. More preferably, the electrolyte is lithium hexafluorophosphate.
In a preferred embodiment of the present invention, the electrolyte is 5 to 20% by mass of the non-aqueous electrolyte solution of the high-voltage lithium ion battery.
The invention also provides a lithium ion battery, which comprises a positive electrode, a diaphragm, a negative electrode and the high-voltage lithium ion battery nonaqueous electrolyte solution as defined in any one of claims 1 to 9.
Preferably, the active material of the positive electrode is lithium cobaltate, lithium manganate, lithium nickel manganese oxide, LiNi1-x-yCoxMnyAlzAnd one or more of manganese-rich solid solutions, wherein x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than or equal to 0 and less than or equal to 1, and x + y + z is more than or equal to 0 and less than or equal to 1.
Preferably, the negative electrode material is one or more of natural graphite, artificial graphite, lithium titanate, a silicon-carbon negative electrode and a silicon negative electrode.
Preferably, the upper limit cut-off voltage of the lithium ion battery is 4.35-5V.
Compared with the prior art, the invention has the advantages that:
1. in the non-aqueous electrolyte of the high-voltage lithium ion battery, the HOMO energy of the silane-based isocyanate additive is higher than that of organic solvents such as EC, the silane-based isocyanate additive preferentially undergoes an oxidation reaction under a high potential, a polymer formed by bond breakage is deposited on the surface of a positive electrode material to become a main component of a CEI film, and the CEI film is a chemically inert protective film layer, so that the catalytic oxidation effect of transition metal ions on the electrolyte can be inhibited, side reactions are inhibited, and the interface of an electrode and the electrolyte is stabilized.
2. In the non-aqueous electrolyte of the high-voltage lithium ion battery, the low-impedance additive can form a uniform and compact SEI film on the surface of the negative electrode, reduce the interface impedance of the negative electrode, and improve the cycle performance and the coulombic efficiency of the battery, thereby greatly prolonging the cycle life at normal temperature.
3. The non-aqueous electrolyte of the high-voltage lithium ion battery can improve the electrochemical performance of the lithium ion battery through the synergistic effect of the components, particularly reduce the impedance and generate gas at high temperature, and greatly improve the cycle life.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail below with reference to examples, it being understood that the following description is only for the purpose of explaining the present invention and is not intended to limit the present invention.
The silane based isocyanate additive structures in the examples and comparative examples are characterized as follows:
compound 1 is represented by the following structural formula:
compound 2 is represented by the following structural formula:
compound 3 has the following structural formula:
compound 4 is represented by the following structural formula:
compound 5 is represented by the following structural formula:
compound 6 has the following structural formula:
compound 7 has the following structural formula:
compound 8 is represented by the following structural formula:
compound 9 has the following structural formula:
compound 10 is represented by the following structural formula:
some of the chemical letters in the examples and comparative examples are abbreviated as follows:
EC (ethylene carbonate), FEC (fluoro)Ethylene carbonate), HFDEC (difluoroethylene carbonate), FEMC (fluoroethylmethyl carbonate), EP (ethyl propionate), D2(1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether), VC (vinylene carbonate), PS (1, 3-propanesultone), DTD (vinyl sulfate), TMSB (tris (trimethylsilane) borate), TMSP (tris (trimethylsilane) phosphate), LiDFP (lithium difluorophosphate), liddob (lithium difluorooxalatoborate), LiBOB (lithium dioxaoxalatoborate), LiBF4Lithium tetrafluoroborate, LiFSI bis (fluorosulfonyl) imide, LiTFSI bis (trifluoromethylsulfonyl) imide.
Example 1
Preparing an electrolyte: in a glove box filled with argon, the oxygen content is less than or equal to 1ppm, the water content is less than or equal to 1ppm, Ethylene Carbonate (EC), fluoroethylene carbonate (FEC), 1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether (D2) are uniformly mixed according to the volume ratio of 30:60:10 to obtain a mixed solution, the compound 1, Vinylene Carbonate (VC) and 1, 3-propane sulfonic acid lactone (PS) are added into the mixed solution, and then lithium hexafluorophosphate (LiPF) is added into the mixed solution6) The solution was completely dissolved by stirring to obtain an electrolyte solution of example 1. Wherein the mass percent of the compound 1 in the electrolyte is 1%, the mass percent of the vinylene carbonate in the electrolyte is 1%, the mass percent of the 1, 3-propane sulfonic lactone in the electrolyte is 1%, and the mass percent of the lithium hexafluorophosphate in the electrolyte is 12.5%.
Examples 2 to 20
Examples 2-20 are also specific examples of electrolyte preparation, and the parameters and preparation method are the same as example 1 except for the parameters in Table 1. The electrolyte formulation is shown in table 1.
Comparative examples 1 to 4
In comparative examples 1 to 4, the parameters and preparation method were the same as in example 1 except for the parameters shown in Table 1. The electrolyte formulation is shown in table 1.
TABLE 1 electrolyte compositions of examples 1 to 20 and comparative examples 1 to 4
Note: the electrolyte concentration is the mass percentage content in the electrolyte;
the content of each component in the silane-based isocyanate additive is the mass percentage content in the electrolyte;
the content of each component in the low-impedance additive is the mass percentage content in the electrolyte;
the proportion of each component in the solvent is volume ratio.
Lithium ion battery performance testing
Preparing a lithium ion battery:
the electrolyte solutions prepared in the examples and comparative examples were injected from LiCoO2And (3) as a positive electrode material, taking graphite as a negative electrode in the lithium ion battery cell, and carrying out processes of packaging, laying aside, formation, aging, secondary packaging, capacity grading and the like after liquid injection is finished to obtain the high-capacity lithium ion battery.
(1) And (3) testing the normal-temperature cycle performance: at 25 ℃, the formed lithium ion battery is charged to 4.5V according to a constant current and a constant voltage of 1C, the current is cut off to 0.02C, and then the lithium ion battery is discharged to 3.0V according to a constant current of 1C. The 600 th cycle capacity retention rate was calculated after 600 cycles of charge/discharge. The calculation formula is as follows:
the 600 th cycle capacity retention rate was 600 th cycle discharge capacity/first cycle discharge capacity × 100%.
(2) High temperature storage performance at 60 ℃: the cell was charged and discharged once at room temperature at 0.5C, the current was cut off at 0.02C and the initial capacity was recorded. Fully filling the battery at a constant current and a constant voltage of 0.5C, and testing the initial thickness and the initial internal resistance of the battery; storing the fully charged battery in a constant temperature environment of 60 ℃ for 28 days, testing the thermal thickness of the battery, and calculating thermal state expansion; and (3) testing the cold thickness, the voltage and the internal resistance after the battery is cooled to the normal temperature for 6 hours, cycling for 3 times according to 0.5C charging and discharging, recording the maximum capacity in the 3 cycles, namely the recovery capacity of the battery, and calculating the residual rate of the battery capacity and the recovery rate of the battery capacity. The calculation formula is as follows:
the thermal state expansion ratio (%) of the battery is (thermal thickness-initial thickness)/initial thickness × 100%;
the change rate (%) of the battery internal resistance is stored internal resistance/initial internal resistance x 100%;
the battery capacity recovery ratio (%) — recovery capacity/initial capacity × 100%.
(3) And (3) testing high-temperature cycle performance: and at the temperature of 45 ℃, the formed lithium ion battery is charged to 4.5V according to a constant current and a constant voltage of 1C, the current is cut off to 0.02C, and then the lithium ion battery is discharged to 3.0V according to a constant current of 1C. The capacity retention rate was calculated at 500 th cycle after 300 cycles of charge/discharge. The calculation formula is as follows:
the 500 th-cycle capacity retention rate was 500 th-cycle discharge capacity/first-cycle discharge capacity × 100%.
TABLE 2 results of cell Performance test of examples 1 to 20 and comparative examples 1 to 4
The reason why the performances of the examples 1 to 20 are obviously superior to those of the comparative example 1 shows that the silyl isocyanate additive can improve the electrochemical performance of the high-voltage LCO/graphite battery, especially reduce the impedance and generate gas at high temperature and improve the high-temperature cycle life is that the silyl isocyanate additive is preferentially oxidized by a solvent at high potential, a polymer formed by bond breaking is deposited on the surface of a positive electrode material to become a main component of a CEI film, the CEI film is uniform and stable in property, side reactions such as catalytic oxidation of electrolyte and the like caused by the dissolution of transition metal ions on the surface of the positive electrode are prevented, and the interface of the electrode and the electrolyte is stabilized.
Comparative examples 3 to 4 were prepared by adding both the silyl isocyanate-based additive represented by structural formula 1 and the low-impedance additive, but the properties were greatly different from those of examples 1 to 20: the silane-based isocyanate additive added too little (comparative example 3) cannot cover the surface of the positive electrode with a protective CEI film, so that the protective effect on the positive electrode is not significant, and the ballooning caused by the decomposition of the electrolyte cannot be suppressed, so that the high-temperature cycle and the high-temperature storage surface are poor. Too much addition (comparative example 4) resulted in excessive growth of the CEI film during cycling, resulting in too much resistance and degraded cycling performance at room temperature. That is, in order to obtain superior battery performance, the silane-based isocyanate additive should be controlled in a suitable amount range.
As can be seen from examples 1-20 and comparative example 2, in comparative example 2, a uniform and compact SEI film is formed on the surface of the negative electrode by adding the low-impedance additive, so that the interfacial impedance of the negative electrode is reduced, the cycle performance and the coulombic efficiency of the battery are improved, and the cycle life at normal temperature is greatly prolonged.
The above is a detailed description of some embodiments of the present invention, and is not intended to limit the scope of the present invention, and any changes or substitutions that do not depart from the gist of the present invention are intended to be within the scope of the present invention.
Claims (10)
1. The non-aqueous electrolyte of the high-voltage lithium ion battery comprises a non-aqueous organic solvent, an electrolyte and an additive, and is characterized in that the additive comprises the following components in percentage by mass in the non-aqueous electrolyte of the lithium ion battery:
silane isocyanate additive 0.1-5%
Low impedance additive 0.1-5%
2. The nonaqueous electrolyte solution for a high-voltage lithium ion battery of claim 1, wherein the silane based isocyanate additive has a structural formula shown in the following formula:
wherein R is1,R2,R3,R4Independently selected from substituted or unsubstituted alkyl group with 1-10 carbon atoms, alkenyl group with 2-10 carbon atoms, C6E10 aralkyl group.
4. the non-aqueous electrolyte solution for high-voltage lithium ion batteries according to claim 1, wherein the low impedance additive is at least one selected from vinylene carbonate, 1, 3-propane sultone, vinyl sulfate, tris (trimethylsilane) borate, tris (trimethylsilane) phosphate, lithium difluorophosphate, lithium difluorooxalate borate, lithium bis-oxalate borate, lithium tetrafluoroborate, lithium bis-sulfonamide imide, and lithium bis (trifluoromethyl) sulfonyl imide.
5. The non-aqueous electrolyte solution for a high-voltage lithium ion battery according to claim 1, wherein the non-aqueous organic solvent is at least one selected from the group consisting of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, ethyl methyl carbonate, methyl propyl carbonate, propyl ethyl carbonate, ethyl acetate, ethyl propionate, ethyl butyrate, propyl acetate, propyl propionate, butyl butyrate, fluoroethylene carbonate, ethylene difluorocarbonate, ethyl fluoroformate, ethyl fluoroacetate, propyl fluoroformate, propyl fluoropropionate, butyl fluoroformate, butyl fluoroacetate, dimethyl sulfone, sulfolane, and 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether.
6. The nonaqueous electrolyte solution for a high-voltage lithium-ion battery according to claim 5, wherein the nonaqueous organic solvent is at least three selected from the group consisting of ethylene carbonate, fluoroethylene carbonate, 1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether, fluoroethylene carbonate, difluoroethylene carbonate and ethyl propionate.
7. The non-aqueous electrolyte solution for a high-voltage lithium ion battery according to claim 1, wherein the electrolyte is at least one of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium difluorophosphate, lithium bis (oxalato) borate, lithium difluorooxalato borate, lithium tetrafluorooxalato phosphate, lithium difluorooxalato phosphate, lithium bis (fluorosulfonyl) imide, lithium bis (trifluoromethanesulfonyl) imide, and lithium fluorosulfonyl (trifluoromethanesulfonyl methyl) imide.
8. The nonaqueous electrolyte solution for a high-voltage lithium-ion battery according to claim 7, wherein the electrolyte is lithium hexafluorophosphate.
9. The non-aqueous electrolyte solution for the high-voltage lithium ion battery as claimed in claim 1, wherein the electrolyte is contained in the non-aqueous electrolyte solution for the high-voltage lithium ion battery in an amount of 5 to 20% by mass.
10. A lithium ion battery comprising a positive electrode, a separator, a negative electrode, and the high-voltage lithium ion battery nonaqueous electrolyte solution according to any one of claims 1 to 9.
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