CN108390098B - High-voltage lithium ion battery electrolyte and high-voltage lithium ion battery - Google Patents
High-voltage lithium ion battery electrolyte and high-voltage lithium ion battery Download PDFInfo
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- CN108390098B CN108390098B CN201810276759.0A CN201810276759A CN108390098B CN 108390098 B CN108390098 B CN 108390098B CN 201810276759 A CN201810276759 A CN 201810276759A CN 108390098 B CN108390098 B CN 108390098B
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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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- 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
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- 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
To overcome the height in the prior artThe invention provides a high-voltage lithium ion battery electrolyte, which comprises lithium salt, solvent and additive, wherein the additive comprises cyclic sultone, fluoro cyclic carbonate, lithium bis-fluoro sulfonyl imide and a compound A shown as the following formula 1: formula 1:
wherein R is1、R2、R3、R4、R5Are each independently selected from-OR6、‑CN、‑NO2、‑F、‑CF3、‑SO3、‑COR7、‑COOR8A hydrocarbon group having 1 to 30 carbon atoms, and R6、R7、R8Each independently selected from a hydrocarbon group having 1 to 30 carbon atoms. Meanwhile, the invention also discloses a lithium ion battery adopting the high-voltage lithium ion battery electrolyte. The high-voltage lithium ion battery electrolyte provided by the invention can obviously reduce the impedance of the battery, improve the low-temperature performance of the battery and improve the high-temperature cycle performance of the battery.
Description
Technical Field
The invention relates to a high-voltage lithium ion battery electrolyte and a high-voltage lithium ion battery using the same.
Background
Lithium ion batteries have a series of advantages of high voltage, high energy and power density, long cycle life, small self-discharge, environmental friendliness and the like, have become the most efficient energy storage devices at present, are widely applied to mobile electronic devices, and are expected to be developed more widely on electric vehicles and hybrid vehicles. With the technological progress and the continuous development of the market, it is increasingly important and urgent to improve the energy density of the lithium battery. In addition to the improvement of the existing materials and the manufacturing process of the battery, the high voltage positive electrode material is one of the more popular research directions, and the high energy density of the battery is realized by increasing the charging depth of the positive electrode active material. To date, a variety of high voltage positive electrode materials such as the binary material LiNiMnO4Ternary material LiNixCoyMnzO2(x + y + z ═ 1), vanadium oxide LiMxV2-xO4And a phosphate-based material LiMPO4Have been successfully developed.
However, the conventional ester electrolyte of the lithium ion battery is easy to cause the problems of impedance increase and great reduction of charge and discharge efficiency of the lithium ion battery under high-temperature voltage, and cannot give consideration to high and low temperature performance, thereby restricting the further development of the high-voltage lithium ion battery.
Disclosure of Invention
The invention aims to solve the technical problem that the high-voltage electrolyte in the prior art has high impedance and cannot give consideration to high and low temperature performances, and provides a high-voltage lithium ion battery electrolyte.
The technical scheme adopted by the invention for solving the technical problems is as follows:
the electrolyte of the high-voltage lithium ion battery comprises a lithium salt, a solvent and an additive, wherein the additive comprises cyclic sultone, fluorinated cyclic carbonate, lithium bis-fluorosulfonyl imide and a compound A shown in the following formula 1:
formula 1:
wherein R is1、R2、R3、R4、R5Are each independently selected from-OR6、-CN、-NO2、-F、-CF3、-SO3、-COR7、-COOR8A hydrocarbon group having 1 to 30 carbon atoms, and R6、R7、R8Each independently selected from a hydrocarbon group having 1 to 30 carbon atoms.
Meanwhile, the invention also provides a high-voltage lithium ion battery, which comprises an anode, a cathode, a diaphragm arranged between the anode and the cathode, and electrolyte, wherein the electrolyte is the high-voltage lithium ion battery electrolyte.
In order to solve the problems of high impedance, poor high-low temperature performance and low capacity retention rate which are easily caused when a high-voltage lithium ion battery is used under higher charge-discharge voltage (not less than 4.25V), the invention uses cyclic sultone, fluorinated cyclic carbonate, lithium bis-fluorosulfonylimide and the compound A shown in the formula 1 in the electrolyte, so that the impedance of the electrolyte is obviously reduced through the synergistic effect of the four substances in an electrolyte system, and the electrolyte has good high-low temperature performance.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects solved by the present invention more apparent, the present invention is further described in detail below with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The high-voltage lithium ion battery electrolyte provided by the invention comprises lithium salt, a solvent and an additive, wherein the additive comprises cyclic sultone, fluorinated cyclic carbonate, lithium bis (fluorosulfonyl) imide and a compound A shown as the following formula 1:
formula 1:
wherein R is1、R2、R3、R4、R5Are each independently selected from-OR6、-CN、-NO2、-F、-CF3、-SO3、-COR7、-COOR8A hydrocarbon group having 1 to 30 carbon atoms, and R6、R7、R8Each independently selected from a hydrocarbon group having 1 to 30 carbon atoms.
In the electrolyte solution, the cyclic sultone is known in the art, and for example, at least one of 1, 3-propane sultone, 1, 4-butane sultone and propenyl-1, 3-sultone can be specifically used, and 1, 3-propane sultone is preferably used.
In the electrolyte provided by the invention, the addition amount of the cyclic sultone can be adjusted in a large range, and preferably, the content of the cyclic sultone is 0.01-5%.
Specifically, one or more of fluoroethylene carbonate, trifluoromethyl ethylene carbonate and difluoroethylene carbonate can be used as the fluorocyclocarbonate. Preferably, the content of the fluorinated cyclic carbonate in the electrolyte solution is 0.01% to 30%, more preferably 0.1% to 3%.
Lithium bis (fluorosulfonyl) imide (LiFSI) is a known substance in the art, and the content of the lithium bis (fluorosulfonyl) imide in the high-voltage lithium ion battery electrolyte provided by the invention is 0.01% -15%.
In the present invention, the compound a is a compound having a structure represented by formula 1, and it is particularly preferable that the compound a is 1-methyl-benzotriazole, because the object of the present invention can be achieved theoretically.
The content of the compound A is 0.01-5%, preferably 0.05-3%, and more preferably 0.1-0.8% based on the total weight of the electrolyte.
The compound A can act together with the cyclic sultone, the fluorinated cyclic carbonate and the lithium bis-fluorosulfonylimide to form a film on the positive and negative electrodes of the battery under high voltage, so that the impedance of the battery is reduced, and the high and low temperature performance of the battery is improved. When the amount of the compound a added is too small, the film forming effect is deteriorated and the battery impedance and high and low temperature performance improving effect is lowered, and when the amount of the compound a added is too high, the battery impedance is increased seriously and the battery performance is deteriorated.
In the high-voltage lithium ion battery electrolyte provided by the invention, under the condition that cyclic sultone, fluorinated cyclic carbonate and lithium bis-fluorosulfonylimide coexist, after the compound A is added, the compound A and the components in the electrolyte generate synergistic action, and the impedance of the battery is unexpectedly and greatly reduced under the condition that the high-temperature and low-temperature performance of the battery is also improved. In addition, in the electrolyte system provided by the invention, the effect of the lithium bis (fluorosulfonyl) imide is also remarkable, and even if the lithium bis (trifluoromethanesulfonyl) imide (LiTFSI) with a similar structure is adopted, the purpose of the invention cannot be achieved, and if the lithium bis (trifluoromethanesulfonyl) imide (LiTFSI) is adopted in an overlarge electrolyte provided by the invention, the cycle performance at high temperature is poor.
According to the invention, in order to achieve a better overall effect, the high-voltage lithium ion battery electrolyte further comprises unsaturated cyclic carbonate. The unsaturated cyclic carbonate is at least one of vinylene carbonate and ethylene carbonate; the content of the unsaturated cyclic carbonate is 0.01-5% by taking the total weight of the electrolyte as a reference.
The high-voltage lithium ion battery electrolyte provided by the invention also comprises a solvent and lithium salt. MakingAs is well known to those skilled in the art, the solvent specific material may be conventional, for example, the lithium salt is selected from LiPF6、LiBF4、LiBOB、LiDFOB、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiC(SO2CF3)3One or more of (a). In the lithium ion battery non-aqueous electrolyte, the content of lithium salt is 0.1-15%. 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, ethyl methyl carbonate and propyl methyl carbonate. The content of the solvent may be adjusted within a wide range, and may be suitably adjusted depending on the content of the various additives and lithium salt as described above.
The invention also provides a high-voltage lithium ion battery, which comprises an anode, a cathode, a diaphragm arranged between the anode and the cathode, and electrolyte, wherein the electrolyte is the electrolyte of the high-voltage lithium ion battery.
Preferably, the positive electrode includes a positive electrode active material, and the active material of the positive electrode is LiNixCoyMnzL(1-x-y-z)O2、LiCox’L(1-x’)O2、LiNix”L’y’Mn(2-x”-y’)O4、Liz’MPO4Wherein L is at least one of Al, Sr, Mg, Ti, Ca, Zr, Zn, Si or Fe, 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, x + y + z is more than or equal to 0 and less than or equal to 1, 0<x ' is not less than 1, x is not less than 0.3 and not more than 0.6, y ' is not less than 0.01 and not more than 0.2, and L ' is at least one of Co, Al, Sr, Mg, Ti, Ca, Zr, Zn, Si and Fe; z' is more than or equal to 0.5 and less than or equal to 1, and M is at least one of Fe, Mn and Co.
The electrolyte provided by the invention is more suitable for a high-voltage lithium ion battery, and preferably, the charge cut-off voltage of the lithium ion battery is more than or equal to 4.25V.
The positive electrode, the negative electrode, and the separator are not specifically limited, and any one of the positive electrode, the negative electrode, and the separator that are conventional in the art may be used.
The present invention will be further illustrated by the following examples.
Examples 1 to 2 and comparative examples 1 to 7
This example illustrates the high voltage lithium ion battery electrolyte disclosed herein.
With LiNi0.5Co0.2Mn0.3O2An artificial graphite electrode material system is used for preparing a 4.35V high-voltage lithium ion battery, which comprises a positive electrode, a negative electrode, a diaphragm arranged between the positive electrode and the negative electrode, and electrolyte, wherein the total weight of the electrolyte is 100%, the electrolyte comprises additive components shown in examples 1-2 and comparative examples 1-7 in the table 1 and the mass percentage of the additive components, and the balance of the components are LiPF6And conventional solvents.
TABLE 1 electrolyte additive composition
The following performance tests were performed on the batteries prepared in the above examples and comparative examples, and the obtained test results were filled in table 2:
(1) and (3) testing high-temperature cycle performance: at 45 ℃, the formed battery is charged to 4.35V by using a 1C constant current and constant voltage, and then discharged to 3.0V by using a 1C constant current. After 300 cycles of charge/discharge, the capacity retention rate at the 300 th cycle was calculated to evaluate the high temperature cycle performance.
The capacity retention rate calculation formula of 300 times of 45 ℃ 1C circulation is as follows:
the 300 th cycle capacity retention (%) (300 th cycle discharge capacity/first cycle discharge capacity) × 100%.
(2) And (3) testing low-temperature discharge performance: at 25 ℃, the formed battery is charged to 4.35V by using a 1C constant current and constant voltage, and then discharged to 3.0V by using a 0.5C constant current, and the discharge capacity is recorded. And then filling the mixture at a constant current and a constant voltage of 1C, placing the mixture in an environment at the temperature of minus 20 ℃ for standing for 12 hours, discharging the mixture at a constant current of 0.5C to 3.0V, and recording the conservation rate of the discharge capacity.
Low-temperature discharge capacity retention rate of-20 ℃ was 0.5C discharge capacity (-20 ℃) and 0.5C discharge capacity (25 ℃)
(3) Testing the performance of normal and low temperature direct current impedance (DCR): the battery 1C after formation was charged to a half-charged state at 25 ℃, charged and discharged for ten seconds with 0.1C, 0.2C, 0.5C, 1C and 2C, respectively, and the charge and discharge cutoff voltages were recorded, respectively. Then, a linear graph (unit: mV) is plotted with the charge and discharge currents of different magnifications as abscissa (unit: A) and the cut-off voltages corresponding to the charge and discharge currents as ordinate.
Charging DCR value is the slope value of a linear plot of different charging currents with corresponding cutoff voltages.
Discharge DCR value is the slope value of a linear plot of different discharge currents with corresponding cutoff voltages.
TABLE 2
Comparing the test results of example 1 and comparative example 5, it can be seen that the addition of 1-methyl-benzotriazole to the electrolyte system containing PS, FEC, LiFIS can significantly reduce DCR while improving high and low temperature performance. While the test results comparing comparative example 4 and comparative examples 1-3 and comparative example 7 and comparative example 6 show that although the addition of 1-methyl-benzotriazole to the PS, FEC or PS, VC system improves the high and low temperature performance and reduces the DCR, the reduction of the DCR is very small.
Comparing the effects of example 1 and example 2, it can be seen that the increase of the content of additives such as 1-methyl-benzotriazole and FEC leads to the decrease of the high temperature performance of the battery, especially the DCR is greatly increased, but the performance is still slightly stronger than that of the electrolyte not containing PS, FEC, LiFIS and 1-methyl-benzotriazole together.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (9)
1. The high-voltage lithium ion battery electrolyte is characterized by comprising a lithium salt, a solvent and an additive, wherein the lithium salt is LiPF6The additive comprises cyclic sultone, fluorinated cyclic carbonate, lithium bis-fluorosulfonylimide and a compound A shown in the following formula 1:
formula 1:
wherein R is1、R2、R3、R4、R5Are each independently selected from-OR6、-CN、-NO2、-F、-CF3、-SO3、-COR7、-COOR8A hydrocarbon group having 1 to 30 carbon atoms, and R6、R7、R8Each independently selected from a hydrocarbon group having 1 to 30 carbon atoms;
the content of the compound A is 0.1-0.8% by taking the total weight of the electrolyte as a reference; the content of the cyclic sultone is 0.01 to 5 percent; the content of the fluorinated cyclic carbonate is 0.1-3%; the content of the lithium bis (fluorosulfonyl) imide is 0.01% -15%.
2. The high voltage lithium ion battery electrolyte of claim 1 wherein the compound a is 1-methyl-benzotriazole.
3. The high voltage lithium ion battery electrolyte of claim 1, wherein the cyclic sultone is selected from at least one of 1, 3-propane sultone, 1, 4-butane sultone, propenyl-1, 3-sultone.
4. The high voltage lithium ion battery electrolyte of claim 1 wherein the fluorinated cyclic carbonate is selected from at least one of fluoroethylene carbonate, trifluoromethyl ethylene carbonate, and difluoroethylene carbonate.
5. The high voltage lithium ion battery electrolyte of claim 1 further comprising an unsaturated cyclic carbonate.
6. The high voltage lithium ion battery electrolyte of claim 5 wherein the unsaturated cyclic carbonate is selected from at least one of vinylene carbonate, ethylene carbonate; the content of the unsaturated cyclic carbonate is 0.01-5% by taking the total weight of the electrolyte as a reference.
7. A high-voltage 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 high-voltage lithium ion battery electrolyte according to any one of claims 1 to 6.
8. The high voltage lithium ion battery of claim 7, wherein the positive electrode comprises a positive active material, the active material of the positive electrode being LiNixCoyMnzL(1-x-y-z)O2、LiCox’L(1-x’)O2、LiNix”L’y’Mn(2-x”-y’)O4、Liz’MPO4Wherein L is at least one of Al, Sr, Mg, Ti, Ca, Zr, Zn, Si or Fe, 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, x + y + z is more than or equal to 0 and less than or equal to 1, 0<x ' is not less than 1, x is not less than 0.3 and not more than 0.6, y ' is not less than 0.01 and not more than 0.2, and L ' is at least one of Co, Al, Sr, Mg, Ti, Ca, Zr, Zn, Si and Fe; z' is more than or equal to 0.5 and less than or equal to 1, and M is at least one of Fe, Mn and Co.
9. The high-voltage lithium ion battery according to claim 7 or 8, wherein the charge cut-off voltage of the high-voltage lithium ion battery is not less than 4.25V.
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| CN112310473A (en) * | 2019-07-30 | 2021-02-02 | 东莞市杉杉电池材料有限公司 | High-low temperature lithium ion battery electrolyte and lithium ion battery |
| CN113871715A (en) * | 2020-06-30 | 2021-12-31 | 诺莱特电池材料(苏州)有限公司 | Lithium iron phosphate battery |
| CN111916826B (en) * | 2020-07-22 | 2021-09-03 | 梅州市量能新能源科技有限公司 | Electrolyte and preparation method thereof, and lithium ion battery and preparation method thereof |
| CN112290095A (en) * | 2020-10-26 | 2021-01-29 | 合肥国轩高科动力能源有限公司 | Lithium ion battery electrolyte suitable for high-nickel material system and preparation method thereof |
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| JP2001143746A (en) * | 1999-11-12 | 2001-05-25 | Denso Corp | Electrolyte for cell and non-aqueous electrolyte secondary cell |
| CN1819324A (en) * | 2006-03-03 | 2006-08-16 | 浙江阻燃锂电材料有限公司 | Electrolyte and lithium ion battery using same |
| CN104638301A (en) * | 2013-11-13 | 2015-05-20 | 浙江省化工研究院有限公司 | High-voltage lithium ion battery electrolyte |
| JP2017152085A (en) * | 2016-02-22 | 2017-08-31 | 旭化成株式会社 | Nonaqueous electrolytic solution and nonaqueous secondary battery |
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| JP2001143746A (en) * | 1999-11-12 | 2001-05-25 | Denso Corp | Electrolyte for cell and non-aqueous electrolyte secondary cell |
| CN1819324A (en) * | 2006-03-03 | 2006-08-16 | 浙江阻燃锂电材料有限公司 | Electrolyte and lithium ion battery using same |
| CN104638301A (en) * | 2013-11-13 | 2015-05-20 | 浙江省化工研究院有限公司 | High-voltage lithium ion battery electrolyte |
| JP2017152085A (en) * | 2016-02-22 | 2017-08-31 | 旭化成株式会社 | Nonaqueous electrolytic solution and nonaqueous secondary battery |
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