CN113258137A - Electrolyte additive for improving electrochemical performance of lithium air battery - Google Patents
Electrolyte additive for improving electrochemical performance of lithium air battery Download PDFInfo
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- CN113258137A CN113258137A CN202110497351.8A CN202110497351A CN113258137A CN 113258137 A CN113258137 A CN 113258137A CN 202110497351 A CN202110497351 A CN 202110497351A CN 113258137 A CN113258137 A CN 113258137A
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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
- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention discloses an electrolyte additive for improving the electrochemical performance of a lithium-air battery, which is a metal heterocyclic compound and a derivative thereof, and has a molecular weight of 800-1500. The invention also provides a high-performance electrolyte containing the electrolyte additive, wherein the high-performance electrolyte can be prepared by adding the additive into a conventional electrolyte, the conventional electrolyte comprises a non-aqueous organic solvent and a lithium salt, the content of the non-aqueous organic solvent is 80-95% of the total weight, the content of the lithium salt is 0.2-5% of the total weight, and the content of the electrolyte additive is 0.1-5% of the total weight; meanwhile, the invention also provides the application of the electrolyte in the lithium air battery, which not only can greatly reduce the overpotential in the charging and discharging process of the lithium air battery and improve the energy efficiency, but also can obviously prolong the cycle life of the lithium air battery; the electrolyte provided by the invention is simple in preparation method and can be prepared in large batch, and the lithium-air battery containing the electrolyte can be stably circulated under a large current.
Description
Technical Field
The invention belongs to the technical field of lithium air batteries, and particularly relates to an electrolyte additive for improving the electrochemical performance of a lithium air battery.
Background
In the past decades, lithium ion batteries have been rapidly developed, have been widely used as main power sources for portable electronic devices such as mobile phones and notebook computers, and have become necessities for human life. However, with the development of high-specific energy devices such as electric vehicles and power grid energy storage, the energy density of the conventional lithium ion battery system operating by the "insertion-extraction" mechanism has been difficult to meet the current market demand. Therefore, the development of new high specific energy storage systems is urgently needed. The lithium-air battery directly adopts metal lithium with the highest theoretical specific capacity (3860mAh/g) and the most negative electrode potential (-3.04V vs. Standard Hydrogen Electrode (SHE)) as a negative electrode and oxygen in the air continuously as an active material of a positive electrode, has the theoretical energy density of about 11680Wh/kg without considering the oxygen quality, can be comparable with gasoline, and is considered as a next-generation high-specific-energy storage system with the most development prospect. However, the complicated reaction history and the delayed multiphase reaction kinetics lead to serious polarization in the charge and discharge process, which causes many problems of low energy efficiency, poor rate capability and cycle performance, and the like, and restricts the commercial application process. Catalysis is key to improving reaction kinetics, and therefore, the design and development of oxygen electrode catalysts are the core problems and research focus of lithium-air batteries.
In order to reduce the charging and discharging overpotential of the lithium air battery, researchers invest a great deal of energy in the aspect of solid-phase oxygen electrode surface catalysis, and develop various solid-phase oxygen electrode catalysts such as carbon materials, noble metals, non-noble metals, composite materials and the like through a series of material design and synthesis methods, and the catalysts effectively improve the reaction kinetics of the lithium air battery, so that the performance of the battery is obviously improved. However, although the solid-phase oxygen electrode catalyst can reduce the charge and discharge overpotential of the lithium air battery to some extent, it has some inherent disadvantages in itself. E.g. with the discharge product Li2O2The solid/solid contact sites between the two are very limited, which limits the catalytic efficiency of the catalyst on one hand and easily causes Li on the other hand2O2Interfacial separation occurs during decomposition, leading to Li2O2The decomposition is incomplete. In order to solve these problems, in recent years, researchers have proposed using a liquid phase additive (also called redox mediator) instead of a solid phase catalyst to reduce the overpotential during charge and discharge. The redox media, such as lithium iodide, tetrathiafulvalene, TEMPO and the like, can be dissolved in the electrolyte, so that the catalyst and Li are greatly increased2O2The contact area of (a). During charging, the redox mediator is first oxidized to the oxidized state and then oxidized to decompose Li2O2And then restores itself to a reduced state. However, the redox mediators reported at present still have some problems, such as that the overpotential during the charge and discharge process is still large, the cycle stability is poor, and the oxidation state of the redox mediator is easy to shuttle to the negative electrode side to react with the lithium metal, so that the lithium metal negative electrode is corroded.
Disclosure of Invention
The invention aims to overcome the defects of the prior art, and provides an electrolyte additive for improving the electrochemical performance of a lithium-air battery aiming at the problems of large charging and discharging overpotential and short cycle life of the lithium-air battery.
In order to achieve the purpose, the invention is realized by the following technical scheme:
the electrolyte additive is a metal heterocyclic compound A and a derivative thereof, the molecular weight of the metal heterocyclic compound A is between 800 and 1500, and the structure of the metal heterocyclic compound A is shown as follows:
further, the derivatives of the metal heterocyclic compound A include B, C, D and the like, B, C and D have the structures shown as follows respectively:
wherein R is1、R2、R3、R4And R5Is a substituent, wherein R1-R5Alternative substituents include alkyl substituents, such as-CH3Methyl, -C2H5Ethyl group, -CH2CH2Ethylene and the like; oxygen-containing substituents, such as-OH hydroxyl, -COOH carboxyl, -CHO aldehyde groups,>c ═ O carbonyl, -OC2H5Ethoxy and the like, -CN cyano and-PPh3Triphenylphosphine, etc., wherein R is1-R5The substituents being selected in accordance with the principle of coordinative bonding, e.g. R attached to C in derivative B, C, D1、R2And R3Is not selected for use>C ═ O carbonyl.
The invention further provides a high-performance electrolyte, which contains the electrolyte additive, wherein the high performance refers to that the charging and discharging overpotential is lower than 0.8V.
Further, the high-performance electrolyte also comprises a non-aqueous organic solvent and a lithium salt, wherein the content of the non-aqueous organic solvent is 80-95% of the total weight of the high-performance electrolyte; the content of lithium salt is 0.2-5% of the total weight of the high-performance electrolyte; the content of the electrolyte additive is 0.1-5% of the total weight of the high-performance electrolyte.
Further, the non-aqueous organic solvent is a sulfone electrolyte (such as dimethyl sulfoxide) or an ether electrolyte (such as tetraethylene glycol dimethyl ether).
Further, the lithium salt is a mixture formed by any one or more of lithium perchlorate, lithium trifluoromethanesulfonate and lithium bistrifluoromethanesulfonimide.
The invention also provides a lithium-air battery, and the electrolyte of the lithium-air battery is the high-performance electrolyte.
Further, the positive electrode material of the lithium-air battery is a composite formed by any one or more of porous carbon, graphene, carbon nanotubes and hollow carbon spheres.
Compared with the prior art, the invention has the following beneficial effects:
1) the invention adopts the metal heterocyclic compound A and the derivative thereof as the electrolyte additive which can promote Li in the discharging process2O2The solution phase growth way of the product reduces the passivation problem of the electrode surface and improves the discharge capacity; the lithium ion battery can be well contacted with a discharge product in the charging process, so that the charging overpotential is effectively reduced; in addition, it can also inhibit the side reaction. The electrolyte additive obviously solves the problems of large charge-discharge polarization and short cycle life of the lithium-air battery, not only reduces the charge-discharge overpotential of the lithium-air battery, but also improves the cycle life of the lithium-air battery.
2) The electrolyte additive has good stability and simple structure, and can be in good contact with a discharge product, so that the decomposition of the discharge product can be efficiently catalyzed.
3) The electrolyte has simple formula and easy preparation, and is beneficial to mass production.
Drawings
Fig. 1 is a schematic diagram comparing electrochemical performance of a high performance electrolyte containing the electrolyte additive of the present invention with that of a conventional electrolyte.
FIG. 2 is a schematic of rate capability of a high performance electrolyte containing the electrolyte additive of the present invention.
Fig. 3 is a schematic of the cycle performance of a high performance electrolyte containing the electrolyte additive of the present invention versus a conventional electrolyte.
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 will be clearly and completely described below with reference to the embodiments of the present invention, and it is obvious that the described embodiments are some embodiments of the present invention, but not all 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.
Example 1
In the lithium-air battery in the embodiment, the positive electrode material is graphene, the negative electrode is metal lithium, the diaphragm is Whatman glass fiber, the high-performance electrolyte containing the electrolyte additive of the invention is used as the electrolyte of the battery, and the usage amount of the electrolyte of each battery is 100 μ L and is about 0.1 g.
The preparation method of the lithium-air battery of the embodiment is as follows:
first, in an argon glove box (H)2O is less than 1ppm) to prepare a conventional electrolyte: adding weighed lithium salt into a nonaqueous organic solvent to obtain a conventional electrolyte, and filling into a clean serum bottle. Then, the electrolyte additive is added into the conventional electrolyte to obtain the high-performance electrolyte.
Wherein the non-aqueous organic solvent is tetraethylene glycol dimethyl ether (TEGDME), and the content of the non-aqueous organic solvent accounts for 94% of the total weight of the high-performance electrolyte; the lithium salt is lithium bis (trifluoromethanesulfonyl) imide (LiITFSI), and the content of the lithium salt accounts for 4% of the total weight of the high-performance electrolyte; the addition of the electrolyte additive is 2% of the total weight of the high-performance electrolyte, the electrolyte additive is a metal heterocyclic compound A, and the structure of the electrolyte additive is as follows:
finally, the lithium-air battery of the present example was assembled with the high-performance electrolyte.
Comparative example
Meanwhile, as a comparative example, a lithium air battery assembled with a conventional electrolyte not containing the electrolyte additive of the present invention was used.
The lithium-air battery of this comparative example and the preparation method thereof are substantially the same as those of example 1, except that the electrolyte used in the lithium-air battery is not added with the electrolyte additive of the present invention, i.e., the conventional electrolyte in example 1 above. Then, a lithium air battery was assembled with the conventional electrolyte.
The assembled lithium air battery in the embodiment 1 and the comparative example is tested for electrochemical performance at room temperature and in a voltage range of 2.0-5.0V.
FIG. 1 is a schematic diagram comparing electrochemical performances of a high-performance electrolyte containing the electrolyte additive of the invention with that of a conventional electrolyte, and it can be seen from the results that the problem of charge-discharge polarization of a lithium air battery can be greatly improved by applying the electrolyte containing the electrolyte additive of the invention, namely, the metal heterocyclic compound A, to the lithium air battery.
FIG. 2 is a schematic diagram showing rate performance of a high-performance electrolyte containing the electrolyte additive of the present invention, and it can be seen from the results that the electrolyte containing the electrolyte additive of the present invention, namely the metal heterocyclic compound A, can obtain better rate performance when used in a lithium air battery.
FIG. 3 is a schematic diagram showing the comparison of the cycle performance of a high performance electrolyte containing the electrolyte additive of the present invention with that of a conventional electrolyte, and it can be seen from the results that the electrolyte containing the electrolyte additive of the present invention, the metal heterocyclic compound A, has a longer cycle life when used in a lithium air battery.
Example 2
This example is substantially the same as example 1 except that the content of the nonaqueous organic solvent tetraethylene glycol dimethyl ether is 95.5% by weight based on the total weight of the high performance electrolyte, and the electrolyte additive is added in an amount of 0.5% by weight based on the total weight of the high performance electrolyte.
Example 3
The difference between this example and example 1 is that the electrolyte additive is a metal heterocyclic compound B, and its structure is shown below:
then, the lithium-air battery of the embodiment is assembled by using the high-performance electrolyte, and the electrochemical performance of the lithium-air battery is tested at room temperature within the voltage range of 2.0-5.0V. The result shows that the electrolyte added with the electrolyte additive metal heterocyclic compound B can reduce the charging and discharging overpotential to 0.4V under the conditions of 100mA/g current density and 1000mAh/g limited capacity for the lithium-air battery, and the charging and discharging overpotential is not obviously attenuated after 30 cycles of circulation.
Example 4
The difference between this example and example 1 is that the electrolyte additive is a metal heterocyclic compound C, and its structure is shown below:
then, the lithium-air battery of the embodiment is assembled by using the high-performance electrolyte, and the electrochemical performance of the lithium-air battery is tested at room temperature within the voltage range of 2.0-5.0V. The result shows that the electrolyte added with the electrolyte additive metal heterocyclic compound C can reduce the charging and discharging overpotential to 0.77V under the conditions of 100mA/g current density and 1000mAh/g limited capacity when being used for the lithium air battery, and the overpotential is not obviously attenuated after 50 cycles of circulation.
Example 5
The difference between this example and example 1 is that the electrolyte additive is a metal heterocyclic compound D, and its structure is shown below:
then, the lithium-air battery of the embodiment is assembled by using the high-performance electrolyte, and the electrochemical performance of the lithium-air battery is tested at room temperature within the voltage range of 2.0-5.0V. The result shows that the electrolyte added with the electrolyte additive metal heterocyclic compound D can reduce the charging and discharging overpotential to 0.41V under the conditions of 100mA/g current density and 1000mAh/g limited capacity when being used for the lithium air battery, and the charging and discharging overpotential is not obviously attenuated after 20 cycles of circulation.
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 (9)
2. the electrolyte additive for improving the electrochemical performance of a lithium-air battery as claimed in claim 1, wherein the derivatives of the metal heterocyclic compound a include B, C and D, and the structures are respectively as follows:
wherein R is1、R2、R3、R4And R5Is a substituent, wherein R1-R5Optional substituents include alkyl substituents, oxygen-containing substituents, -CN and-PPh3。
3. The electrolyte additive for improving the electrochemical performance of a lithium-air battery as claimed in claim 1 or 2, wherein the molecular weight of the metal heterocyclic compound is 800-1500.
4. A high performance electrolyte, characterized in that the electrolyte contains the electrolyte additive according to claim 2.
5. The high-performance electrolyte of claim 4, further comprising a non-aqueous organic solvent and a lithium salt, wherein the content of the non-aqueous organic solvent is 80-95% of the total weight of the high-performance electrolyte; the content of lithium salt is 0.2-5% of the total weight of the high-performance electrolyte; the content of the electrolyte additive is 0.1-5% of the total weight of the high-performance electrolyte.
6. The high-performance electrolyte according to claim 4, wherein the non-aqueous organic solvent is a sulfone electrolyte or an ether electrolyte.
7. The high-performance electrolyte solution of claim 4, wherein the lithium salt is a mixture of any one or more of lithium perchlorate, lithium trifluoromethanesulfonate and lithium bistrifluoromethanesulfonimide.
8. A lithium-air battery, characterized in that, the electrolyte of the lithium-air battery is the high-performance electrolyte of any one of claims 4-7.
9. The lithium-air battery according to claim 8, wherein the positive electrode material of the lithium-air battery is a composite formed by any one or more of porous carbon, graphene, carbon nanotubes and hollow carbon spheres.
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