CN113346133A - All-weather high-rate lithium battery electrolyte and lithium ion battery - Google Patents
All-weather high-rate lithium battery electrolyte and lithium ion battery Download PDFInfo
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- CN113346133A CN113346133A CN202110413533.2A CN202110413533A CN113346133A CN 113346133 A CN113346133 A CN 113346133A CN 202110413533 A CN202110413533 A CN 202110413533A CN 113346133 A CN113346133 A CN 113346133A
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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
- H01M10/05—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
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- H01M10/0569—Liquid materials characterised by the solvents
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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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Abstract
The invention provides an all-weather high-rate lithium battery electrolyte and a lithium ion battery, wherein the lithium battery electrolyte comprises a lithium salt electrolyte, an organic solvent and an additive, wherein the freezing point of the organic solvent is-150 to-20 ℃; the additive is one or more of lithium nitrate, lithium perchlorate, lithium sulfate and lithium carbonate, and the mass content of the additive in the lithium battery electrolyte is 0.1-10%. The electrolyte provided by the invention has the advantages that the melting point of each component is low, the viscosity is small, the conductivity is high, and the high conductivity is still kept at low temperature even from minus 60 ℃ to minus 100 ℃, so that the cycle performance of the ternary lithium battery under the extreme low temperature condition is greatly improved. The invention can also greatly improve the oxidation resistance of the electrolyte, broaden the electrochemical window of the electrolyte and form a stable SEI film, thereby being suitable for the efficient operation of the ternary cathode material under the high voltage of 4.2-4.5V.
Description
Technical Field
The invention relates to the technical field of electrochemistry, in particular to all-weather high-rate lithium battery electrolyte and a lithium ion battery.
Background
Batteries are used as devices capable of storing and continuously providing electric energy, and continuously meet the requirements of people on flexible application of electric power. Among many battery systems, lithium ion batteries have been widely accepted by the market due to their excellent performance, and have been applied to the fields of consumer electronics, new energy vehicles and energy storage on a large scale since the commercialization of the japan SONY company in 1991, and have become indispensable important components for various products.
However, the lithium ion battery based on the commercial carbonate electrolyte has the problems of reduced discharge voltage platform, low discharge capacity, fast capacity attenuation, poor rate capability and the like in a low-temperature environment, so that the lithium ion battery cannot operate at a temperature lower than-20 ℃, and the application of the lithium ion battery in the fields of special equipment, aerospace, polar investigation, cold zone emergency rescue and the like is severely limited.
In recent years, researchers have conducted a great deal of research. It is reported in the literature that the use of liquefied gas in place of electrolyte allows the lithium battery to operate efficiently at-60 c, but the performance of the battery at room temperature still needs to be improved and a special high pressure vessel is required to keep the liquefied gas in a liquid state. There is also a report on reduction of the affinity between a solvent and lithium ions by dissolving a fluorine-containing electrolyte into a highly fluorinated nonpolar solvent, the electrolyte having high electrochemical stability over a wide voltage range (0.0 to 5.6V) and LiNi even at a low temperature of-85 DEG C0.8Co0.15Al0.05O2The | Li battery can still provide about 50% of room temperature capacity; but the conductivity of the electrolyte system is lower at low temperature (-80 ℃, 0.011mS cm)-1) Long cycle performance at ultra-low temperatures is unknown, while highly fluorinated solvents are generally toxic and expensive, and are not suitable for large-scale production and application. CN103078141A discloses a lithium ion secondary battery electrolyte, which contains a solvent, a lithium salt and a film forming additive, the technical scheme adopts the combination of linear carboxylic ester and ethylene carbonate to obtain a solvent system with high dielectric constant and low viscosity, but the capacity retention rate of the solvent system at-20 ℃ is only 40-45%, the low-temperature performance is not ideal, and the use requirement under the low-temperature condition cannot be met. CN 108270033A adds functional auxiliary agents of fluoroethylene carbonate and propenyl-1, 3-propane sultone in a LiBOB and LiODFB lithium salt system, thereby reducing the interface impedance of the electrolyte and improving the low-temperature performance of the lithium ion battery, although the scheme is in generalityThe battery performance is improved under the low-temperature environment condition, but the problem of low lithium salt conductivity can not be solved under the ultralow temperature condition of 50 ℃ below zero.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides an all-weather high-rate lithium battery electrolyte and a lithium ion battery, which realize excellent charge and discharge performance in various climatic environments at low cost and have higher practical application value.
The invention adopts the following technical scheme:
the invention provides an all-weather high-rate lithium battery electrolyte, which comprises a lithium salt electrolyte, an organic solvent and an additive,
wherein the freezing point of the organic solvent is-150 to-20 ℃;
the additive is one or more of lithium nitrate, lithium perchlorate, lithium sulfate and lithium carbonate, and the mass content of the additive in the lithium battery electrolyte is 0.1-10%.
The lithium ion battery of the traditional carbonate electrolyte has the problems of reduced discharge voltage platform, low discharge capacity, fast capacity attenuation, poor rate performance and the like at low temperature, although researchers propose various improvement methods, the problems are still difficult to solve simultaneously, and more or less new problems are brought in. The research of the invention finds that by adding a certain amount of the additive into an organic solvent with a freezing point of-150 to-20 ℃, the double electric layer structure of an interface of a positive electrode and an electrolyte can be greatly changed to form a highly crosslinked solvated layer, so that the oxidation resistance of the electrolyte can be improved, the electrochemical window of the electrolyte can be widened, and a stable SEI film can be formed, further the electrolyte not only has higher conductivity below 0 ℃ (especially under the ultralow temperature condition of-60 to 100 ℃), the normal operation of the circulation of a ternary lithium battery under high voltage (4.2 to 4.5V) is ensured, the service life and the energy density of the lithium battery under the ultralow temperature extreme condition are greatly improved, and the lithium battery also has high power density within the range of room temperature to-100 ℃.
Preferably, the organic solvent is one or more of diethyl ether, ethylene glycol dimethyl ether, triethylene glycol dimethyl ether, tetraethylene glycol dimethyl ether, 1, 3-dioxolane, tetrahydrofuran and methyl tetrahydrofuran.
Preferably, the lithium salt electrolyte is lithium bis (fluorosulfonylimide) (LiFSI), lithium bis (trifluoromethylsulfonyl imide) (LiTFSI), lithium (triflate) (LiSO)3CF3) Lithium tetrafluoroborate (LiBF)4) And lithium bis (oxalato) borate (LiBOB).
Preferably, the concentration of the lithium salt electrolyte is 0.01-5 mol/L.
In a preferred embodiment of the invention, the lithium salt electrolyte is lithium bis (trifluoromethyl) sulfonyl imide, the organic solvent is ethylene glycol dimethyl ether, and the additive is lithium perchlorate, wherein the mass content of the additive in the lithium battery electrolyte is 0.6-1.2%.
In another preferred embodiment of the invention, the lithium salt electrolyte is lithium bis (trifluoromethyl) sulfonyl imide, the organic solvent is composed of tetrahydrofuran and methyltetrahydrofuran, wherein the volume ratio of the methyltetrahydrofuran in the organic solvent is 0-20%, and the additive is lithium nitrate, and the mass content of the additive in the lithium battery electrolyte is 0.6-1.2%.
The invention also provides a lithium ion battery which comprises the lithium battery electrolyte. The lithium ion battery provided by the invention is not limited in form and can be a cylinder, an aluminum shell, a plastic shell or a soft package shell.
Further, the lithium ion battery also comprises a positive electrode, a negative electrode and a diaphragm arranged between the positive electrode and the negative electrode. The positive electrode can be lithium iron phosphate, lithium cobaltate or a ternary positive electrode material, and preferably is a ternary positive electrode material. For example LiNixCoyMn1-x-yO2Wherein x is more than 0 and less than 1, y is more than 0 and less than 1, and x + y is less than 1.
Furthermore, the charging upper limit voltage of the lithium ion battery is more than or equal to 4.2V and less than or equal to 4.5V.
The invention provides all-weather high-rate lithium battery electrolyte and a lithium ion battery, and the electrolyte provided by the invention has the advantages that the melting point of each component is low, the viscosity is small, the conductivity is high, and the high conductivity is still kept at low temperature even at-60 ℃ to-100 ℃, so that the cycle performance of a ternary lithium battery under an extremely low temperature condition is greatly improved. The invention can also greatly improve the oxidation resistance of the electrolyte, broaden the electrochemical window of the electrolyte and form a stable SEI film, thereby being suitable for the efficient operation of the ternary cathode material under the high voltage of 4.2-4.5V.
Drawings
FIG. 1 is a graph of normal temperature cycle performance of a battery prepared from the electrolyte of example 3 of the present invention;
FIG. 2 is a graph of the low temperature cycling performance of a battery made from the electrolyte of example 3 of the invention;
fig. 3 is a graph of different temperature discharge curves for batteries prepared from the electrolyte of example 3 of the present invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention are clearly and completely described below, and it is obvious that the described embodiments are a part of the embodiments of the present invention, but not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Unless otherwise specified, the technical means used in the examples of the present invention are conventional means well known to those skilled in the art.
The components used in the following examples and comparative examples are of battery grade.
The electrolyte in the following examples was formulated under conditions such that the electrolyte was operated in a glove box filled with argon gas having a purity of 99.999% and having a moisture content of less than 0.1ppm and a temperature of room temperature.
Example 1
This embodiment provides an electrolyte for a lithium battery, which is prepared as follows:
and (3) in a glove box filled with argon, fully mixing 143g of lithium bis (trifluoromethyl) sulfonyl imide, 500mL of ethylene glycol dimethyl ether and 20g of lithium nitrate, and uniformly stirring to obtain the lithium ion battery.
Example 2
This embodiment provides an electrolyte for a lithium battery, which is prepared as follows:
and (3) in a glove box filled with argon, taking 93.5g of lithium bis (fluorosulfonyl) imide, 250mL of ethylene glycol dimethyl ether, 250mL of 1, 3-dioxolane and 6g of lithium nitrate, fully mixing, and uniformly stirring to obtain the lithium ion battery.
Example 3
This embodiment provides an electrolyte for a lithium battery, which is prepared as follows:
and (3) in a glove box filled with argon, taking 143g of bis (trifluoromethyl) sulfimide lithium, 500mL of ethylene glycol dimethyl ether and 6g of lithium perchlorate, fully mixing, and uniformly stirring to obtain the lithium ion battery.
Example 4
This embodiment provides an electrolyte for a lithium battery, which is prepared as follows:
and (3) in a glove box filled with argon, fully mixing 143g of lithium bis (trifluoromethyl) sulfonyl imide, 500mL of tetrahydrofuran and 6g of lithium nitrate, and uniformly stirring to obtain the lithium ion battery.
Example 5
This embodiment provides an electrolyte for a lithium battery, which is prepared as follows:
and (3) in a glove box filled with argon, fully mixing 143g of lithium bis (trifluoromethyl) sulfonyl imide, 400mL of tetrahydrofuran, 100mL of methyltetrahydrofuran and 6g of lithium nitrate, and uniformly stirring to obtain the lithium bis (trifluoromethyl) sulfonyl imide.
Comparative example 1
This comparative example provides a lithium battery electrolyte, which was formulated as follows:
and (3) in a glove box filled with argon, taking 143g of lithium bistrifluoromethylsulfonyl imide and 500mL of ethylene glycol dimethyl ether, fully mixing, and uniformly stirring to obtain the lithium bis (trifluoromethyl) sulfonyl imide.
Comparative example 2
This comparative example provides a lithium battery electrolyte, which was formulated as follows:
and (3) in a glove box filled with argon, taking 152g of lithium hexafluorophosphate, 500mL of ethylene carbonate and 500mL of diethyl carbonate, fully mixing, and uniformly stirring to obtain the lithium hexafluorophosphate ethylene carbonate.
Comparative example 3
This comparative example provides a lithium battery electrolyte, which was formulated as follows:
and (3) in a glove box filled with argon, fully mixing 143g of lithium bis (trifluoromethyl) sulfonyl imide, 500mL of tetrahydrofuran and 6g of lithium tetrafluoroborate, and uniformly stirring to obtain the lithium tetrafluoroborate.
Comparative example 4
This comparative example provides a lithium battery electrolyte, which was formulated as follows:
and (3) in a glove box filled with argon, fully mixing 143g of bis (trifluoromethyl) sulfimide lithium, 500mL of ethylene glycol dimethyl ether and 6g of lithium trifluoromethanesulfonate, and uniformly stirring to obtain the lithium trifluoromethanesulfonate.
Comparative example 5
This comparative example provides a lithium battery electrolyte, which was formulated as follows:
in a glove box filled with argon, 287g of lithium bis (trifluoromethyl) sulfonyl imide, 500mL of ethylene glycol dimethyl ether, 500mL of 1, 3-dioxolane and 15g of potassium bromide are fully mixed and stirred uniformly to obtain the lithium ion battery.
Performance testing
The electrolytes prepared in each example and comparative example are respectively assembled into a battery and then subjected to cycle performance test, and the method comprises the following steps: with LiNi0.8Co0.1Mn0.1O2(NCM811) is a positive electrode, a lithium sheet is a negative electrode, an aluminum foil is a current collector, a Celgard2325 diaphragm is adopted as the diaphragm, a button half cell is assembled in a glove box, and the test is carried out after standing. The battery was activated at room temperature of 25C with charging and discharging at 1/5C 3.0V to 4.3V, and then discharged at different temperatures at 1/10C, respectively, and the test results are shown in table 1. The charge and discharge cycles at room temperature 25 ℃ and at-20 ℃ were carried out at 1/2C, and the test results are shown in Table 2.
FIG. 1 is a graph of the normal temperature 25 ℃ cycling performance of a battery prepared from the electrolyte of example 3;
FIG. 2 is a graph of the low temperature-20 ℃ cycling performance of a battery prepared from the electrolyte of example 3; fig. 3 is a graph of different temperature discharge curves for batteries prepared from the electrolyte of example 3.
TABLE 1 discharge Capacity of different cells at different temperatures
TABLE 2 results of charge-discharge cycles at 25 deg.C and-20 deg.C of different batteries at 1/2C
In tables 1 and 2, a capacity of 0 means that the battery cannot be cycled under high voltage without suitable additives.
Finally, it should be noted that: the above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention.
Claims (10)
1. An all-weather high-rate lithium battery electrolyte is characterized by comprising a lithium salt electrolyte, an organic solvent and an additive,
wherein the freezing point of the organic solvent is-150 to-20 ℃;
the additive is one or more of lithium nitrate, lithium perchlorate, lithium sulfate and lithium carbonate, and the mass content of the additive in the lithium battery electrolyte is 0.1-10%.
2. The all-weather high-rate lithium battery electrolyte as claimed in claim 1, wherein the organic solvent is one or more of diethyl ether, ethylene glycol dimethyl ether, triethylene glycol dimethyl ether, tetraethylene glycol dimethyl ether, 1, 3-dioxolane, tetrahydrofuran, and methyl tetrahydrofuran.
3. The all-weather, high-rate lithium battery electrolyte of claim 1 or 2, wherein the lithium salt electrolyte is one or more of lithium bis-fluorosulfonylimide, lithium bis-trifluoromethylsulfonyl imide, lithium triflate, lithium tetrafluoroborate and lithium bis-oxalato borate.
4. The all-weather high-rate lithium battery electrolyte as claimed in claim 3, wherein the concentration of the lithium salt electrolyte is 0.01-5 mol/L.
5. The all-weather high-rate lithium battery electrolyte as claimed in any one of claims 1 to 4, wherein the lithium salt electrolyte is lithium bis (trifluoromethylsulfonyl) imide,
the organic solvent is glycol dimethyl ether,
the additive is lithium perchlorate, and the mass content of the additive in the lithium battery electrolyte is 0.6-1.2%.
6. The all-weather high-rate lithium battery electrolyte as claimed in any one of claims 1 to 4, wherein the lithium salt electrolyte is lithium bis (trifluoromethylsulfonyl) imide,
the organic solvent consists of tetrahydrofuran and methyltetrahydrofuran, wherein the volume of the methyltetrahydrofuran in the organic solvent accounts for 0-20%,
the additive is lithium nitrate, and the mass content of the additive in the lithium battery electrolyte is 0.6-1.2%.
7. A lithium ion battery comprising the lithium battery electrolyte according to any one of claims 1 to 6.
8. The lithium ion battery of claim 7, further comprising a positive electrode, a negative electrode, and a separator disposed between the positive electrode and the negative electrode, wherein the positive electrode is a ternary positive electrode material.
9. The lithium of claim 8The ion battery is characterized in that the ternary positive electrode material is LiNixCoyMn1-x- yO2Wherein x is more than 0 and less than 1, y is more than 0 and less than 1, and x + y is less than 1.
10. The lithium ion battery according to any one of claims 7 to 9, wherein the upper limit charge voltage of the lithium ion battery is 4.2V or more and 4.5V or less.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN115995610A (en) * | 2023-03-22 | 2023-04-21 | 河北省科学院能源研究所 | High-performance lithium ion battery electrolyte and preparation method and application thereof |
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| CN108336397A (en) * | 2018-02-07 | 2018-07-27 | 清华大学 | A kind of ether-ether composite electrolyte for stablizing lithium metal battery |
| CN109802181A (en) * | 2019-02-21 | 2019-05-24 | 中国科学院青岛生物能源与过程研究所 | A kind of double main salt electrolyte of the wide temperature window for lithium battery |
| CN112490507A (en) * | 2020-12-04 | 2021-03-12 | 苏州大学张家港工业技术研究院 | Lithium-sulfur battery electrolyte and preparation method and application thereof |
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Patent Citations (4)
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| CN1964123A (en) * | 2005-11-10 | 2007-05-16 | 比亚迪股份有限公司 | A non-aqueous electrolyte for lithium cell |
| CN108336397A (en) * | 2018-02-07 | 2018-07-27 | 清华大学 | A kind of ether-ether composite electrolyte for stablizing lithium metal battery |
| CN109802181A (en) * | 2019-02-21 | 2019-05-24 | 中国科学院青岛生物能源与过程研究所 | A kind of double main salt electrolyte of the wide temperature window for lithium battery |
| CN112490507A (en) * | 2020-12-04 | 2021-03-12 | 苏州大学张家港工业技术研究院 | Lithium-sulfur battery electrolyte and preparation method and application thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN115995610A (en) * | 2023-03-22 | 2023-04-21 | 河北省科学院能源研究所 | High-performance lithium ion battery electrolyte and preparation method and application thereof |
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