CN116315102A - Nonaqueous electrolyte and sodium ion battery - Google Patents
Nonaqueous electrolyte and sodium ion battery Download PDFInfo
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- CN116315102A CN116315102A CN202310365404.XA CN202310365404A CN116315102A CN 116315102 A CN116315102 A CN 116315102A CN 202310365404 A CN202310365404 A CN 202310365404A CN 116315102 A CN116315102 A CN 116315102A
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- sodium
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- nonaqueous
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- ion battery
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
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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 provides a non-aqueous electrolyte and a sodium ion battery. The nonaqueous electrolyte comprises a nonaqueous organic solvent, electrolyte salt and an additive, wherein the additive comprises a compound I and/or a compound II. The compound I and the compound II have sodium-sulfur bonds, the structure is very stable, and a solid electrolyte interface (CEI) film can be formed on the surface of the anode through reduction, so that the high-temperature performance of the battery is improved. The nitrogenous five-membered heterocyclic compound can be used as a stabilizer of electrolyte salt (especially sodium hexafluorophosphate) in the electrolyte, and can reduce side reactions of the battery caused by decomposition of the electrolyte, thereby improving the stability of the electrolyte. The two functional groups are bonded together through a carbon-sulfur covalent bond C-S, so that soluble sulfide is not easy to generate in the discharging process, and the dissolving capacity of SEI/CEI components can be reduced, so that the cycle life and the high-temperature storage performance of the battery are improved by reducing the decomposition of electrolyte in the circulating and storing processes.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to a nonaqueous electrolyte and a sodium ion battery.
Background
Along with the new energy vehicle entering the explosion period, the price of lithium ores is increased greatly, the price of lithium carbonate is increased by 10 times within two years, and the development space of the lithium ion battery is limited finally due to the fact that the cost of the lithium battery is greatly increased to bring larger pressure to an industrial chain. From a resource reserve perspective, lithium resources are increasingly scarce, while sodium resources are more 1353 times more abundant in the crust than lithium resources. In the same main group, sodium and lithium have similar physical and chemical properties, and have wide application prospects in the fields of large-scale energy storage, electric vehicles, electric ships, special engineering vehicles and the like due to the advantages of abundant sodium resources, low price, environmental friendliness and the like. The working principle of the sodium ion battery is similar to that of a lithium ion battery, and the sodium ion battery is mainly relied on to be detached and embedded back and forth between the anode and the cathode. However, as the ionic radius of sodium ions is larger than that of lithium ions, and the common negative electrode material has large specific surface area of hard carbon and smaller interlayer spacing, so that sodium ions are difficult to separate after being intercalated, the sodium ions are irreversibly consumed, the content of sodium ions capable of freely moving is reduced, and the problems of low primary efficiency, poor high-temperature storage performance and the like of the full battery are caused.
In addition, the ideal SEI film formed by the additives in the electrolyte should be electronically insulating and ionically conductive, insoluble and inert with respect to the electrolyte to avoid irreversible capacity loss from side reactions. In SEI film formed in sodium ion battery, compared to lithium ion batterySolubility of alkyl sodium and alkyl sodium carbonate in carbonate is higher than that of inorganic NaF and Na 2 CO 3 The equivalent height is 70-80 times, and the inorganic component NaF and Na in the Na-SEI 2 CO 3 Compared with the inorganic component LiF and Li in the Li-SEI 2 CO 3 The solubility of the sodium-ion battery is 30-40 times higher, the instability of Na-SEI is caused, and the side reaction with electrolyte is increased, so that the high-temperature storage and the cycle performance of the sodium-ion battery are reduced.
Accordingly, there is a need to develop a novel solvent or additive to form a less soluble SEI component to reduce the occurrence of side reactions.
Disclosure of Invention
In view of the above problems, an object of the present invention is to provide a nonaqueous electrolyte solution and a sodium ion battery, in which an additive contained in the nonaqueous electrolyte solution has a stable structure and can form a stable CEI film, and in which side reactions of the electrolyte solution can be reduced and the stability thereof can be improved, so that the cycle life and high-temperature storage performance of the sodium ion battery can be improved.
To achieve the above object, a first aspect of the present invention provides a nonaqueous electrolytic solution comprising a nonaqueous organic solvent, an electrolyte salt and an additive comprising compound I and/or compound II,
the electrolyte used in the invention comprises a compound I and/or a compound II. The compound I and the compound II have sodium-sulfur bonds, the structure is very stable, and a solid electrolyte interface (CEI) film can be formed on the surface of the anode through reduction, so that the high-temperature performance of the battery is improved. In addition, the nitrogenous five-membered heterocyclic compound can be used as a stabilizer of electrolyte salt (especially sodium hexafluorophosphate) in the electrolyte, so that side reactions of the battery caused by decomposition of the electrolyte are reduced, and the stability of the electrolyte is improved. The two functional groups are bonded together through a carbon-sulfur covalent bond C-S, so that soluble sulfide is not easy to generate in the discharging process, and the dissolving capacity of SEI/CEI components can be reduced, so that the cycle life and the high-temperature storage performance of the battery are improved by reducing the decomposition of electrolyte in the circulating and storing processes.
As one technical scheme of the invention, the sum of the mass of the nonaqueous organic solvent, the electrolyte salt and the additive is m, and the mass of the additive is n, and n/m is 0.01-2.00%.
As a technical scheme of the invention, n/m is 0.01-0.50%.
As a technical scheme of the invention, the electrolyte salt accounts for 6.5-15.5% of the sum of the mass of the nonaqueous organic solvent, the mass of the electrolyte salt and the mass of the additive.
As an aspect of the present invention, the electrolyte salt is a sodium salt selected from at least one of sodium hexafluorophosphate, sodium perchlorate, sodium tetrafluoroborate, sodium trifluoromethylsulfonate, sodium bistrifluoromethylsulfonylimide, sodium bisoxalato borate, sodium difluorophosphate, sodium difluorooxalato borate, sodium difluorodioxaato phosphate, and sodium difluorosulfonylimide.
As an embodiment of the present invention, the nonaqueous organic solvent is at least one of a chain carbonate, a cyclic carbonate and a carboxylic acid ester.
As an aspect of the present invention, the nonaqueous organic solvent is at least one selected from the group consisting of ethylene carbonate, dimethyl carbonate, diethyl carbonate, ethylmethyl carbonate, propylene carbonate, butyl acetate, propyl propionate, ethyl propionate and ethyl butyrate.
The second aspect of the present invention provides a sodium ion battery comprising a positive electrode material, a negative electrode material, and a nonaqueous electrolyte. The sodium ion battery has better cycle life and high-temperature storage performance, and is favorable for further industrialized development of the sodium ion battery.
As one technical scheme of the invention, the positive electrode material is a layered oxide, and the chemical formula of the layered oxide is Na x M (1-y-z) Fe y Mn z O 2 Wherein M is selected from at least one of Co, ni, cu, mg, zn, al, sn, ga, cr, sr, V and Ti, 0<x≤1，0≤y<1，0≤z<1，y+z≤1。
As an aspect of the present invention, the negative electrode material is at least one selected from a carbon-based negative electrode material, a titanium-based oxide negative electrode material, and an alloy-based negative electrode material.
Detailed Description
The invention mainly provides a nonaqueous electrolyte for a sodium ion battery. Of course, the sodium ion battery may include a positive electrode material and a negative electrode material in addition to the nonaqueous electrolytic solution.
The positive electrode material can be a layered oxide, and the chemical formula of the layered oxide is Na x M (1-y-z) Fe y Mn z O 2 Wherein M is selected from at least one of Co, ni, cu, mg, zn, al, sn, ga, cr, sr, V and Ti, 0<x≤1，0≤y<1，0≤z<1, y+z is less than or equal to 1. Of course, the positive electrode material may be other materials capable of generating ion deintercalation with sodium ions. The anode material is selected from at least one of a carbon-based anode material, a titanium-based oxide anode material, and an alloy-based anode material. Further, the negative electrode material may be selected from hard carbon, soft carbon, sodium titanate, sb alloy, sn alloy, potassium alloy, aluminum alloy, copper alloy, molybdenum alloy, and the like. Wherein, soft carbon can be graphitized into amorphous carbon at a high temperature of more than 2500 ℃, and even though hard carbon is processed at a high temperature, the graphitization phenomenon is difficult to occur, and the hard carbon has stronger sodium storage capacity and lower working potential.
The nonaqueous electrolytic solution of the present invention may include an electrolyte salt, a nonaqueous organic solvent and an additive.
Wherein the electrolyte salt accounts for 6.5 to 15.5 percent of the sum of the mass of the nonaqueous organic solvent, the electrolyte salt and the additive. . Preferably, the electrolyte salt is 8-15%. As an example, the electrolyte salt may be 6.5%, 7.0%, 7.5%, 8.0%, 8.5%, 9.0%, 10.0%, 10.5%, 11.0%, 11.5%, 12.0%, 12.5%, 13.0%, 13.5%, 14.0%, 14.5%, 15.0%, 15.5% in ratio, but is not limited thereto. The electrolyte salt is sodium salt selected from sodium hexafluorophosphate (NaPF) 6 ) Sodium perchlorate (NaClO) 4 ) Sodium tetrafluoroborate (NaBF) 4 ) Sodium triflate (NaCF) 3 SO 3 ) Sodium bistrifluoromethylsulfonylimide (NaN (CF) 3 SO 2 ) 2 ) Sodium bisoxalato borate (C) 4 BLiO 8 ) Sodium difluorophosphate (NaPO) 2 F 2 ) Sodium difluorooxalato borate (C) 2 BF 2 NaO 4 ) At least one of sodium difluorodioxalate phosphate (NaDFBP) and sodium difluorosulfimide (NaFSI).
The nonaqueous organic solvent accounts for 80% or more, preferably 85% or more of the total mass of the nonaqueous organic solvent, the electrolyte salt and the additive. The nonaqueous organic solvent is at least one of a chain carbonate, a cyclic carbonate and a carboxylic acid ester. Preferably, the nonaqueous organic solvent is a mixture of a chain carbonate and a cyclic carbonate. As an example, the nonaqueous organic solvent is selected from at least one of Ethylene Carbonate (EC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethylmethyl carbonate (EMC), propylene Carbonate (PC), butyl acetate (n-Ba), γ -butyrolactone (γ -Bt), propyl propionate (n-Pp), ethyl Propionate (EP), and ethyl butyrate (Eb). Preferably, the nonaqueous organic solvent is a combination of ethylene carbonate (PC), ethylmethyl carbonate (EMC) and diethyl carbonate (DEC) to achieve a more stable cycle performance.
The additives may include compound I and/or compound II.
The additive accounts for 0.01 to 2.00 percent of the sum of the mass of the nonaqueous organic solvent, the electrolyte salt and the additive. Preferably, the additive accounts for 0.01 to 0.50 percent of the sum of the mass of the nonaqueous organic solvent, the electrolyte salt and the additive. By way of example, the additive may be, but is not limited to, 0.01%, 0.02%, 0.03%, 0.04%, 0.05%, 0.08%, 0.10%, 0.20%, 0.30%, 0.40%, 0.50%, 0.60%, 0.70%, 0.80%, 0.90%, 1.00%, 1.10%, 1.20%, 1.30%, 1.40%, 1.50%, 1.60%, 1.70%, 1.80%, 1.90%, 2.00%.
For a better description of the objects, technical solutions and advantageous effects of the present invention, the present invention will be further described with reference to specific examples. It should be noted that the following implementation of the method is a further explanation of the present invention and should not be taken as limiting the present invention.
Wherein, the specific conditions are not noted in the examples, and the method can be carried out according to the conventional conditions or the conditions suggested by manufacturers. The reagents or apparatus used were conventional products available commercially without the manufacturer's attention.
Example 1
(1) Preparation of nonaqueous electrolyte: preparing an electrolyte in a vacuum glove box with the water content less than 1ppm under the argon atmosphere, mixing ethylene carbonate EC, propylene carbonate PC, methyl ethyl carbonate EMC and diethyl carbonate DEC according to the weight ratio of EC: PC: EMC: DEC=5:25:30:40 in the glove box with the dried argon atmosphere, adding a compound I (CAS: 51138-06-8) additive, dissolving and fully stirring, adding sodium hexafluorophosphate, and uniformly mixing to obtain the electrolyte.
(2) Preparation of positive electrode: ternary material NaNi of sodium nickel cobalt aluminate 1/3 Fe 1./3 Mn 1/3 O 2 Uniformly mixing the adhesive PVDF and the conductive agent SuperP according to the mass ratio of 95:1:4 to prepare sodium ion battery anode slurry with certain viscosity, coating the mixed slurry on two sides of an aluminum foil, and drying and rolling to obtain the anode plate.
(3) Preparation of the negative electrode: preparing slurry from hard carbon, a conductive agent SuperP, a thickener CMC and an adhesive SBR (styrene butadiene rubber emulsion) according to the mass ratio of 95:1.5:1.0:2.5, uniformly mixing, coating the mixed slurry on two sides of a copper foil, and drying and rolling to obtain the negative plate.
(4) Preparation of sodium ion battery: and (3) preparing the positive plate, the diaphragm and the negative plate into square cells in a lamination mode, packaging by adopting polymers, filling the prepared nonaqueous electrolyte of the sodium ion battery, and preparing the sodium ion battery with the capacity of 1400mAh through the procedures of formation, capacity division and the like.
The electrolyte formulations of examples 1 to 12 and comparative examples 1 to 3 are shown in Table 1, and the procedure for preparing the electrolytes and preparing the batteries of examples 2 to 12 and comparative examples 1 to 3 is the same as that of example 1.
Table 1 electrolyte components of examples and comparative examples
The sodium ion batteries manufactured in examples 1 to 12 and comparative examples 1 to 3 were respectively subjected to a high temperature storage performance test, a high temperature cycle test and a safety test under the following specific test conditions, and the test results are shown in table 2.
(1) Sodium ion battery high temperature storage test
Charging and discharging the sodium ion battery at 0.5C/0.5C once (the discharge capacity of the battery is recorded as C0) under the condition of normal temperature (25 ℃), and the upper limit voltage is 4.0V; placing the battery in a 60 ℃ oven for 30d, taking out the battery, placing the battery in a 25 ℃ environment, discharging at 0.5 ℃, and recording the discharge capacity as C1; the sodium ion cell was then charged and discharged once at 0.5C/0.5C (cell discharge capacity is reported as C2).
Capacity retention = (C1/C0) ×100%
Capacity recovery = (C2/C0) ×100%
(2) High temperature cycle test of sodium ion battery
And placing the sodium ion battery in a 45 ℃ incubator, and standing for 30min to keep the sodium ion battery at a constant temperature. The first-turn discharge capacity of the battery was recorded as one charge-discharge cycle by charging with a constant current of 1C to a voltage of 4.0V, then charging with a constant voltage of 4.0V to a current of 0.05C, and then discharging with a constant current of 1C to a voltage of 2.0V. The cycle was continued for 400 weeks, and the discharge capacity of the first cycle and the discharge capacity of the last cycle were recorded, and the capacity retention was calculated as follows.
Capacity retention = last cycle discharge capacity/first cycle discharge capacity x 100%
(3) Sodium ion battery safety performance test
And (3) placing the sodium ion battery in a 60 ℃ oven, heating to 60 ℃ at a heating speed of 5 ℃/min, keeping the temperature at 60 ℃ for 30min, carrying out 1C constant-current constant-voltage charging on the sodium ion battery, wherein the upper limit voltage is 10V, and observing whether the battery has serious swelling, smoking, fire, explosion and other phenomena.
Table 2 results of performance testing of sodium ion batteries of various examples
As can be seen from the results of Table 2, the sodium ion batteries of examples 1 to 12 were better in high-temperature storage performance, high-temperature cycle performance and safety performance than those of comparative examples 1 to 3. This is because the compounds I and II used in examples 1 to 12 have sodium-sulfur bonds, and the structure is very stable, and a solid electrolyte interface (CEI) film can be formed by reduction on the surface of the anode, thereby improving the high temperature performance of the battery. In addition, the nitrogenous five-membered heterocyclic compound can be used as a stabilizer of electrolyte salt (especially sodium hexafluorophosphate) in the electrolyte, so that side reactions of the battery caused by decomposition of the electrolyte are reduced, and the stability of the electrolyte is improved. The two functional groups are bonded together through a carbon-sulfur covalent bond C-S, so that soluble sulfide is not easy to generate in the discharging process, and the dissolving capacity of SEI/CEI components can be reduced, so that the cycle life and the high-temperature storage performance of the battery are improved by reducing the decomposition of electrolyte in the circulating and storing processes.
Compound III of comparative example 2 has phenyl group, has a large steric hindrance, and has a large battery impedance, which is unfavorable for high-temperature cycle performance. In comparative example 3, sodium-sulfur bond is not present but sulfur-hydrogen bond is present, hydrogen bond is active, and side reaction of electrolyte is difficult to be suppressed, so that the performance of sodium-ion battery is not good.
As is clear from comparative examples 1 to 5 or comparative examples 6 to 10, the sodium ion battery is more excellent in performance when the compound I and/or the compound II account for 0.01 to 0.50% by mass of the nonaqueous electrolytic solution.
Comparative examples 1 to 10 show that the sodium ion battery containing compound II is better in high-temperature storage performance and high-temperature cycle performance than the sodium ion battery containing compound I because the compound II also has a sulfonic acid group, which generates lower impedance of organic/inorganic components during the reaction, and which increases more slowly during long-term cycle, thus exhibiting excellent cycle performance.
Comparative examples 4, 9 and 11 show that the sodium ion battery performs better when the additive contains both compound I and compound II due to the synergistic effect between the two.
Finally, it should be noted that the above embodiments are only for illustrating the technical solution of the present invention and not for limiting the scope of the present invention, and although the present invention has been described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that the present invention can be modified or substituted without departing from the spirit and scope of the technical solution of the present invention.
Claims (10)
1. A nonaqueous electrolyte solution comprising a nonaqueous organic solvent, an electrolyte salt and an additive, characterized in that the additive comprises a compound I and/or a compound II,
2. the nonaqueous electrolytic solution according to claim 1, wherein a sum of mass of the nonaqueous organic solvent, the electrolyte salt and the additive is m, and a mass of the additive is n, and n/m is 0.01 to 2.00%.
3. The nonaqueous electrolytic solution according to claim 2, wherein n/m is 0.01 to 0.50%.
4. The nonaqueous electrolytic solution according to claim 1, wherein the electrolyte salt is 6.5 to 15.5% of the sum of the mass of the nonaqueous organic solvent, the mass of the electrolyte salt and the mass of the additive.
5. The nonaqueous electrolytic solution according to claim 4, wherein the electrolyte salt is a sodium salt selected from at least one of sodium hexafluorophosphate, sodium perchlorate, sodium tetrafluoroborate, sodium trifluoromethylsulfonate, sodium bistrifluoromethylsulfonylimide, sodium bisoxalato borate, sodium difluorophosphate, sodium difluorooxalato borate, sodium difluorobisoxalato phosphate and sodium bisfluorosulfonyl imide.
6. The nonaqueous electrolytic solution according to claim 1, wherein the nonaqueous organic solvent is at least one of a chain carbonate, a cyclic carbonate and a carboxylic acid ester.
7. The nonaqueous electrolytic solution according to claim 6, wherein the nonaqueous organic solvent is at least one selected from the group consisting of ethylene carbonate, dimethyl carbonate, diethyl carbonate, methylethyl carbonate, propylene carbonate, butyl acetate, propyl propionate, ethyl propionate and ethyl butyrate.
8. A sodium ion battery comprising a positive electrode material, a negative electrode material and the nonaqueous electrolytic solution according to any one of claims 1 to 7.
9. The sodium ion battery of claim 8, wherein the positive electrode material is a layered oxide having a chemical formula Na x M (1-y-z) Fe y Mn z O 2 Wherein M is selected from at least one of Co, ni, cu, mg, zn, al, sn, ga, cr, sr, V and Ti, 0<x≤1，0≤y<1，0≤z<1，y+z≤1。
10. The sodium ion battery of claim 8, wherein the negative electrode material is selected from at least one of a carbon-based negative electrode material, a titanium-based oxide negative electrode material, and an alloy-based negative electrode material.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN116895839A (en) * | 2023-08-29 | 2023-10-17 | 合肥市赛纬电子材料有限公司 | Nonaqueous electrolyte and sodium ion battery containing same |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN116895839A (en) * | 2023-08-29 | 2023-10-17 | 合肥市赛纬电子材料有限公司 | Nonaqueous electrolyte and sodium ion battery containing same |
| CN116895839B (en) * | 2023-08-29 | 2024-04-05 | 合肥市赛纬电子材料有限公司 | Nonaqueous electrolyte and sodium ion battery containing same |
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