CN113675471A - Battery electrolyte and battery comprising same - Google Patents
Battery electrolyte and battery comprising same Download PDFInfo
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- CN113675471A CN113675471A CN202110924198.2A CN202110924198A CN113675471A CN 113675471 A CN113675471 A CN 113675471A CN 202110924198 A CN202110924198 A CN 202110924198A CN 113675471 A CN113675471 A CN 113675471A
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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
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2200/00—Safety devices for primary or secondary 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
- H01M2300/0088—Composites
- H01M2300/0091—Composites in the form of mixtures
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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 battery electrolyte and a battery containing the same, wherein the battery electrolyte comprises an electrolyte, an organic solvent and a composite functional additive; the composite functional additive comprises nitrate and/or nitrite, and also comprises 1, 4-dioxane and/or 1, 3-dioxolane. In the invention, nitrate and/or nitrite is used to cooperate with 1, 4-dioxane and/or 1, 3-dioxolane as a composite functional additive, so that the cycle performance, low-temperature performance and safety performance of the battery can be improved. Particularly, for the lithium ion battery with the negative electrode material of graphite, the composite material of monocrystalline silicon and graphite or the composite material of silicon monoxide and graphite, the capacity retention rate in the full cycle life stage can be improved, so that the lithium ion battery has high safety, excellent cycle stability and excellent low-temperature performance.
Description
Technical Field
The invention belongs to the technical field of electrochemical energy storage, and relates to a battery electrolyte and a battery comprising the same.
Background
Currently, organic electrolyte materials used in the lithium battery industry are mainly alkyl carbonate compounds and LiPF6Lithium salt system, the performance of which is greatly reduced at high temperature (above 60 ℃), while the power battery for electric automobile requires a higher working temperature range (about-30 to 80 ℃); moreover, the alkyl carbonate organic electrolyte material has high flammability, so that the safety has great hidden trouble; especially in the field of hybrid and all-electric automotive applications, long-term cycling problems and safety are important factors that limit the practical application of these materials.
The electrolyte is an important component of the lithium ion battery, and plays a role in transmitting lithium ions between the positive electrode and the negative electrode. The safety, charge-discharge cycle, working temperature range and charge-discharge capacity of the battery are all important in relation to the electrochemical performance of the electrolyte. The traditional functional components in the electrolyte play a key role in prolonging the service life of the battery, but no long-term effective measure is provided for delaying or inhibiting the generation of lithium dendrites, so that the safety performance of the battery and the service life of charge-discharge cycles are greatly influenced.
Xin Zhang et al reported that 1, 4-dioxane can inhibit side reactions on the surface of lithium metal when applied to a lithium air battery. Shuhong Jiao et al reported that lithium nitrate applied to a battery using lithium metal as a negative electrode can improve the coulombic efficiency, high-temperature cycle performance and low-temperature performance of the lithium metal battery. Their research results mainly focused on batteries with lithium metal as the negative electrode, mainly revealing the role of a single component; it is not disclosed in graphite, Si/C, SiOxand/C and the like.
Disclosure of Invention
In view of the shortcomings of the prior art, the present invention provides a battery electrolyte and a battery comprising the same.
In order to achieve the purpose, the invention adopts the following technical scheme:
in one aspect, the present invention provides a battery electrolyte comprising an electrolyte, an organic solvent, and a complex-function additive; the composite functional additive comprises nitrate and/or nitrite, and also comprises 1, 4-dioxane and/or 1, 3-dioxolane.
In the invention, nitrate and/or nitrite is used to cooperate with 1, 4-dioxane and/or 1, 3-dioxolane as a composite functional additive, so that the cycle performance, low-temperature performance and safety performance of the battery can be improved. Particularly, for the lithium ion battery with the negative electrode material of graphite, the composite material of monocrystalline silicon and graphite or the composite material of silicon monoxide and graphite, the capacity retention rate at the full cycle life stage can be improved, and the cycle performance, the low-temperature performance and the safety performance of the battery can be improved.
If only 1, 4-dioxane and/or 1, 3-dioxolane is added into the electrolyte, the capacity retention rate of the battery in early circulation can be improved, but the capacity retention rate of the battery in long-term circulation is not assisted. When only nitrate and/or nitrite is added into the electrolyte, the capacity retention rate of the battery in long-term circulation can be improved, but the capacity retention rate of the battery in early-stage circulation is not assisted. The capacity retention rate of the battery at the full cycle life stage can be improved by combining the two types of substances.
Preferably, the nitrate is any one of lithium nitrate, sodium nitrate or magnesium nitrate or a combination of at least two of them.
Preferably, the nitrite is any one of lithium nitrite, sodium nitrite or magnesium nitrite or a combination of at least two thereof.
Preferably, the nitrate and/or nitrite is present in an amount of 0.01% to 5%, for example 0.01%, 0.05%, 0.08%, 0.1%, 0.5%, 0.8%, 1%, 2%, 3%, 4% or 5% by mass, based on 100% by mass of the total battery electrolyte.
Preferably, the 1, 4-dioxane or/and 1, 3-dioxolane is present in an amount of 0.2 to 20% by mass, for example 0.2%, 0.5%, 0.8%, 1%, 3%, 5%, 8%, 10%, 12%, 14%, 16%, 18% or 20% by mass, based on 100% by mass of the total mass of the battery electrolyte.
Preferably, the electrolyte is a lithium salt.
Preferably, the lithium salt comprises LiClO4、LiPF6、LiBF4、LiTFSI、LiFSI、LiBOB、LiODFB、LiCF3SO3Or LiAsF6Any one or a combination of at least two of them.
Preferably, the electrolyte is present in an amount of 8% to 49% by mass, for example 8%, 10%, 13%, 15%, 18%, 20%, 23%, 25%, 28%, 30%, 35%, 38%, 40%, 44% or 49% by mass, based on 100% by mass of the total battery electrolyte.
Preferably, the organic solvent is at least one of carbonate, halogenated carbonate, carboxylate, propionate, fluoroether, aromatic hydrocarbon or halogenated aromatic hydrocarbon.
Preferably, the halogen in the halogenated carbonate or the halogenated aromatic hydrocarbon is at least one of F, Cl, Br or I.
Preferably, the carbonate comprises one or a combination of at least two of ethylene carbonate, propylene carbonate, diethyl carbonate, dimethyl carbonate or ethyl methyl carbonate.
Preferably, the halogenated carbonate includes at least one of fluoroethylene carbonate (FEC), difluoroethylene carbonate (DFEC), propylene carbonate difluoride, ethyl trifluoroacetate, trifluoroethyl methyl carbonate, trifluoromethyl ethylene carbonate, 4-trifluoromethyl ethylene carbonate, vinyl chlorocarbonate, bis (2,2, 2-trifluoroethyl) carbonate, methyl trifluoropropionate, ethyl 3,3, 3-trifluoroacetate, methyl 2- (trifluoromethyl) benzoate, ethyl 4,4, 4-trifluorobutyrate, or 1,1,1,3,3, 3-hexafluoroisopropyl acrylate, or a combination of at least two thereof.
Preferably, the carboxylic acid ester includes one or a combination of at least two of propyl butyrate, propyl acetate, isopropyl acetate, butyl propionate, isopropyl propionate, ethyl butyrate, methyl propionate (EM), Ethyl Propionate (EP), Propyl Propionate (PP), and the like.
Preferably, the fluoroether is an ether having 7 or less carbon atoms in the molecule.
Preferably, the halogenated aromatic hydrocarbon is one or a combination of at least two of monofluorobenzene, difluorobenzene, 1,3, 5-trifluorobenzene, trifluorotoluene, 2-fluorotoluene or 2, 4-dichlorotrifluorotoluene.
In the present invention, the organic solvent may be one or a combination of at least two of Ethylene Carbonate (EC), Propylene Carbonate (PC), diethyl carbonate (DEC), dimethyl carbonate (DMC), Ethyl Methyl Carbonate (EMC), fluoroethylene carbonate (FEC), Propyl Acetate (PA), isopropyl acetate (IPA), methyl propionate (EM), Ethyl Propionate (EP), Propyl Propionate (PP), Butyl Propionate (BP), isopropyl propionate (IPP), Ethyl Butyrate (EB), or Propyl Butyrate (PB).
Preferably, the total mass percentage of organic solvent in the battery electrolyte is 51% to 92%, such as 51%, 53%, 55%, 60%, 65%, 68%, 70%, 75%, 78%, 80%, 85%, 88% or 90%.
In another aspect, the present invention provides a lithium ion battery comprising the battery electrolyte as described above.
Preferably, the battery is a lithium ion battery, a potassium ion battery, a sodium ion battery or a magnesium ion battery.
Preferably, in the invention, the negative electrode material of the lithium ion battery suitable for being matched with the electrolyte is graphite, or a composite material of monocrystalline silicon and graphite, or a composite material of silicon oxide and graphite, or lithium titanate, or Nb2O5。
Preferably, the graphite is artificial graphite or natural graphite.
Compared with the prior art, the invention has the following beneficial effects:
in the invention, nitrate and/or nitrite is used to cooperate with 1, 4-dioxane and/or 1, 3-dioxolane as a composite functional additive, so that the cycle performance, low-temperature performance and safety performance of the battery can be improved. Particularly, for the lithium ion battery with the negative electrode material of graphite, the composite material of monocrystalline silicon and graphite or the composite material of silicon monoxide and graphite, the capacity retention rate in the full cycle life stage can be improved, so that the lithium ion battery has high safety, excellent cycle stability and excellent low-temperature performance.
Drawings
Fig. 1 is a graph showing the results of a capacity retention rate test at the full cycle life stage of lithium ion batteries containing the electrolytes of example 1, comparative example 1, and comparative example 2.
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.
The general test platform used in examples 1 to 5, and comparative examples 1 to 3 is as follows:
the positive electrode adopts a binder PVDF-S5130, a composite conductive agent Super-P/KS-6 (the mass ratio of Super-P: KS-6 is 2: 1), a nickel cobalt lithium manganate (NCM622) ternary positive electrode material and a solvent NMP (N-methyl-2-pyrrolidone, N-methyl pyrrolidone), the negative electrode adopts artificial graphite (the model is fir P15), conductive agents Super-P solvent CMC, H2O and a binder SBR as raw materials, the wet pulping process is respectively adopted to prepare slurry, the viscosity of the positive electrode is adjusted to 10000-13000 mPa.s, the viscosity of the negative electrode is adjusted to 1500-3000 mPa.s, the N/P ratio is designed to be 1.12, the capacity is 1671mAh, the slurry is prepared by coating, slicing, rolling, splitting, drying at 140 ℃ for 8H, pasting an adhesive tape, winding a battery core and drying at 80 ℃ for 48H, and then the lithium ion battery is laid for 24H according to the following different electrolyte formulas, And preparing the lithium ion soft package battery by formation, primary final sealing, aging and secondary final sealing, and then testing the cycle performance and the safety performance of the battery. The compositions of the electrolytes of examples 1 to 5 and comparative examples 1 to 3 are shown in Table 1.
TABLE 1
The cycle performance and safety performance of the lithium ion battery prepared by using the NCM622 nickel-cobalt-manganese ternary material as the cathode material and using the electrolyte formulations of examples 1 to 5 and comparative examples 1 to 3 were tested, and the test results are shown in the following tables 2, 3 and 4:
TABLE 2 Normal temperature cycle capacity retention ratio of the battery
TABLE 3 high temperature cycling capacity retention of the battery at 55 deg.C
TABLE 4(-20 ℃ discharge rate)
| Distinguishing | Example 1 | Example 2 | Example 3 | Example 4 | Example 5 | Comparative example 1 | Comparison ofExample 2 | Comparative example 3 |
| Discharge rate at-20 ℃ 1C | 86.3％ | 86.2％ | 85.9％ | 86.6％ | 86.1％ | 80.2％ | 81.2％ | 68.3％ |
The general test platform used in example 6 and comparative example 4 (electrolyte compositions are shown in table 5) is as follows:
the positive electrode adopts a binder PVDF-S5130, a composite conductive agent Super-P/KS-6 (the mass ratio of Super-P: KS-6 is 2: 1), a lithium cobaltate positive electrode material, a solvent NMP (N-methyl-2-pyrrolidone), and a negative electrode SiOxThe method comprises the steps of taking a/C material (fibrate S420), a conductive agent Super-P solvent CMC, H2O and a binder SBR as raw materials, preparing slurry by adopting a wet pulping process respectively, adjusting the viscosity of a positive electrode to 10000-13000 mPa & S, adjusting the viscosity of a negative electrode to 1500-3000 mPa & S, designing the N/P ratio to be 1.12 and the capacity to 1860mAh, preparing the lithium ion soft package battery by coating, slicing, rolling, splitting, drying at 140 ℃ for 8H, sticking an adhesive tape, winding the battery core and drying at 80 ℃ for 48H, preparing the lithium ion soft package battery by injecting and sealing the lithium ion battery according to different electrolyte formulas, standing for 24H, forming, carrying out primary final sealing, aging and secondary final sealing, and testing the cycle performance and the safety performance of the battery, wherein the testing results are shown in tables 6-8.
TABLE 5
TABLE 6 Normal temperature cycle capacity retention ratio of the battery
TABLE 7 high temperature cycle capacity retention of the battery at 55 deg.C
TABLE 8(-20 ℃ discharge rate)
| Distinguishing | Example 6 | Comparative example 4 |
| Discharge rate at-20 ℃ 1C | 84.5％ | 67.2％ |
The general test platform used in example 7 and comparative example 5 (electrolyte compositions are shown in table 9) is as follows:
the positive electrode adopts a binder PVDF-S5130, a composite conductive agent Super-P/KS-6 (the mass ratio of Super-P: KS-6 is 2: 1), a nickel-cobalt sodium manganate (NCM523) ternary positive electrode material and a solvent NMP (N-methyl-2-pyrrolidone, N-methyl pyrrolidone), the negative electrode adopts artificial graphite (the model is fir P15), a conductive agent Super-P solvent, H2O and a binder SBR as raw materials, the wet pulping process is respectively adopted to prepare slurry, the viscosity of the positive electrode is adjusted to 10000-13000 mPa.s, the viscosity of the negative electrode is adjusted to 1500-3000 mPa.s, the N/P ratio is designed to be 1.12, the capacity is 1463mAh, the slurry is subjected to coating, slicing, rolling, splitting, drying at 140 ℃ for 8H, liquid adhesive tape pasting, battery winding and drying at 80 ℃ for 48H, and then the lithium ion battery is laid aside according to the following different electrolyte formulas, Forming, primary final sealing, aging and secondary final sealing to prepare the lithium ion soft package battery, and then testing the cycle performance and the safety performance of the battery, wherein the test results are shown in tables 10-11.
TABLE 9
TABLE 10 Normal temperature cycle capacity retention ratio of the battery
TABLE 11 high temperature cycling capacity retention of the battery at 55 ℃
In summary, it can be seen that the use of nitrate and/or nitrite, and 1, 4-dioxane and/or 1, 3-dioxolane significantly improves the charge-discharge cycle performance and low-temperature discharge performance of the battery using graphite or silicon-containing material as the negative electrode.
Fig. 1 is a graph showing the results of a capacity retention rate test at the full cycle life stage of a lithium ion battery containing the electrolytes of example, comparative example 1 and comparative example 2, and it can be seen from fig. 1 that when only 1, 4-dioxane and/or 1, 3-dioxolane is added to the electrolyte, it has an effect of improving the capacity retention rate of the battery at the early cycle, but does not contribute to the capacity retention rate of the battery at the long-term cycle. When only nitrate and/or nitrite is added into the electrolyte, the capacity retention rate of the battery in long-term circulation can be improved, but the capacity retention rate of the battery in early-stage circulation is not assisted. The electrolyte of example 1 can improve the capacity retention rate of the battery at the full cycle life stage.
The applicant states that the present invention is illustrated by the above examples of the battery electrolyte and the battery comprising the same, but the present invention is not limited to the above examples, i.e. it is not meant that the present invention must be implemented by means of the above examples. It will be apparent to those skilled in the art that any modification of the present invention, equivalent substitutions of selected materials and additions of auxiliary components, selection of specific modes and the like, which are within the scope and disclosure of the present invention, are contemplated by the present invention.
Claims (10)
1. The battery electrolyte is characterized by comprising an electrolyte, an organic solvent and a composite functional additive; the composite functional additive comprises nitrate and/or nitrite, and also comprises 1, 4-dioxane and/or 1, 3-dioxolane.
2. The battery electrolyte of claim 1, wherein the nitrate is any one of lithium nitrate, sodium nitrate, or magnesium nitrate, or a combination of at least two thereof;
preferably, the nitrite is any one of lithium nitrite, sodium nitrite or magnesium nitrite or a combination of at least two thereof.
3. The battery electrolyte according to claim 1 or 2, wherein the nitrate and/or nitrite is present in an amount of 0.01 to 5% by mass, based on 100% by mass of the total battery electrolyte.
4. The battery electrolyte as claimed in any of claims 1 to 3, wherein the 1, 4-dioxane or/and 1, 3-dioxolane is present in an amount of from 0.2 to 20% by mass, based on 100% by mass of the total mass of the battery electrolyte.
5. The battery electrolyte of any of claims 1-4, wherein the electrolyte is a lithium salt.
6. The battery electrolyte of claim 5, wherein the lithium salt comprises LiClO4、LiPF6、LiBF4、LiTFSI、LiFSI、LiBOB、LiODFB、LiCF3SO3Or LiAsF6Any one or a combination of at least two of them.
7. The battery electrolyte as claimed in any of claims 1 to 6, wherein the electrolyte is present in an amount of 8 to 49% by mass, based on 100% by mass of the total mass of the battery electrolyte.
8. The battery electrolyte of any of claims 1-7, wherein the organic solvent is at least one of a carbonate, a halogenated carbonate, a carboxylate, a propionate, a fluoroether, an aromatic hydrocarbon, or a halogenated aromatic hydrocarbon;
preferably, the halogen in the halogenated carbonate or the halogenated aromatic hydrocarbon is at least one of F, Cl, Br or I;
preferably, the carbonate comprises one or a combination of at least two of ethylene carbonate, propylene carbonate, diethyl carbonate, dimethyl carbonate or ethyl methyl carbonate;
preferably, the halogenated carbonate includes at least one of fluoroethylene carbonate, difluoroethylene carbonate, difluoropropylene carbonate, trifluoroethyl acetate, trifluoroethyl methyl carbonate, trifluoromethyl ethylene carbonate, 4-trifluoromethylethylene carbonate, chloroethylene carbonate, bis (2,2, 2-trifluoroethyl) carbonate, methyl trifluoropropionate, ethyl 3,3, 3-trifluoroacetate, methyl 2- (trifluoromethyl) benzoate, ethyl 4,4, 4-trifluorobutyrate, or 1,1,1,3,3, 3-hexafluoroisopropyl acrylate or a combination of at least two thereof;
preferably, the carboxylic acid ester comprises one or a combination of at least two of propyl butyrate, propyl acetate, isopropyl acetate, butyl propionate, isopropyl propionate, ethyl butyrate, methyl propionate, ethyl propionate, or propyl propionate;
preferably, the fluoroether is an ether having 7 or less carbon atoms in the molecule;
preferably, the halogenated aromatic hydrocarbon is one or a combination of at least two of monofluorobenzene, difluorobenzene, 1,3, 5-trifluorobenzene, trifluorotoluene, 2-fluorotoluene or 2, 4-dichlorotrifluorotoluene.
9. The battery electrolyte of claim 8, wherein the total mass percent of organic solvent in the battery electrolyte is between 51% and 92%.
10. A battery comprising the battery electrolyte of any one of claims 1-15;
preferably, the battery is a lithium ion battery, a sodium ion battery or a magnesium ion battery;
preferably, the negative electrode material of the lithium ion battery is graphite, or a composite material of monocrystalline silicon and graphite, or a composite material of silicon oxide and graphite, or lithium titanate, or Nb2O5；
Preferably, the graphite is artificial graphite or natural graphite.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114865080A (en) * | 2022-04-02 | 2022-08-05 | 香河昆仑新能源材料股份有限公司 | Lithium ion battery electrolyte and lithium ion battery |
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| CN114865080A (en) * | 2022-04-02 | 2022-08-05 | 香河昆仑新能源材料股份有限公司 | Lithium ion battery electrolyte and lithium ion battery |
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