CN113823839B - Electrolyte and sodium ion battery containing same - Google Patents
Electrolyte and sodium ion battery containing same Download PDFInfo
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- CN113823839B CN113823839B CN202111256126.1A CN202111256126A CN113823839B CN 113823839 B CN113823839 B CN 113823839B CN 202111256126 A CN202111256126 A CN 202111256126A CN 113823839 B CN113823839 B CN 113823839B
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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
-
- 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
- H01M10/0569—Liquid materials characterised by the solvents
-
- 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
-
- 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 application provides an electrolyte and a sodium ion battery containing the same. The electrolyte of the present application includes at least: a base ether solvent; long-chain ether solvent tetraethylene glycol dimethyl ether; a sodium salt; a first additive and a second additive; the first additive is a vulcanization accelerator; the second additive is a nitrile material. The sodium ion electrolyte provided by the application has high electrochemistry and long cycle life. The sodium ion electrolyte provided by the application has the advantages of simple preparation process, high yield and low cost, is suitable for industrial application, and has a wide application prospect in the fields of portable electronic equipment and power batteries.
Description
Technical Field
The application belongs to the field of sodium ion batteries, and relates to an electrolyte and a sodium ion battery containing the same.
Background
Lithium ion batteries are widely used in portable electronic products such as mobile phones, notebook computers and the like, electric tools, electric bicycles and electric automobiles, and greatly change living habits and production modes of people. The high-voltage high-energy-density high-energy-efficiency hybrid power supply has irreplaceable functions. With the rapid growth of electric vehicles and large-scale energy storage demands, lithium consumption has been and continues to increase rapidly. However, the abundance of lithium element in the crust is very low and the global distribution is very uneven, which severely restricts the development of electric vehicles and large-scale energy storage.
Sodium with similar physical and chemical properties to lithium is relatively abundant in the crust and widely distributed, and has a similar deintercalation mechanism to lithium, reversible circulation in an electrode material can be realized, the theoretical specific capacity of metal sodium is 1166mAh/g, and the metal sodium is lower than that of a lithium ion battery, but can replace part of application scenes of the lithium ion battery, such as a large-scale energy storage system with lower energy density requirements, so that research and development of the sodium ion secondary battery is expected to alleviate the problem caused by lithium resource shortage to a certain extent.
Sodium ion batteries have developed rapidly in recent years and have been considered as one of the most potential solutions for low cost large scale energy storage systems. The research and development experience of other systems such as lithium ion batteries is referenced and borrowed, and the research and development of novel anode and cathode materials of sodium ion batteries are rapid. However, as a battery component which is important as an electrode material, development of a novel electrolyte is not active nor mature, which directly affects effective exertion of electrochemical properties of the electrode material and stable and safe operation of the battery. Sodium ions and ether solvent molecules in ether electrolyte are attracting more and more attention and research because intercalation reaction can occur in graphite with high reversibility and stable electrode/electrolyte interface is effectively constructed on the surface of the cathode material. However, the research of the ether electrolyte in the sodium ion battery is relatively preliminary, and the long-cycle requirement of the sodium ion battery still cannot be met at present.
Disclosure of Invention
In view of the above, the present application provides an electrolyte and a sodium ion battery comprising the same. The electrolyte disclosed by the application uses the vulcanization accelerator, the reaction energy barrier of the vulcanization accelerator is low, the electron obtaining capability is strong, and the film is easy to form on the surface of the negative electrode; the vulcanization accelerator has oxidation-reduction property, can promote the oxidation of the anode, and is beneficial to constructing a stable electrode electrolyte interface; the tetraethylene glycol dimethyl ether in the electrolyte has high solvation capacity for free sodium ion salt, and is beneficial to solvation of sodium ions in the electrolyte; the vulcanization accelerator in the electrolyte can complex anions in part of the electrolyte with the nitrile material, and the tetraethylene glycol dimethyl ether is favorable for solvating sodium salt, and the nitrile material is also favorable for improving the conductivity of the electrolyte.
In order to achieve the above purpose, the present application adopts the following technical scheme:
the application provides an electrolyte, which at least comprises the following components: a base ether solvent; long-chain ether solvent tetraethylene glycol dimethyl ether; a sodium salt; a first additive and a second additive; the first additive is a vulcanization accelerator; the second additive is a nitrile material.
The inventor finds that the tetraethylene glycol dimethyl ether has high solvating capability for free sodium ion salt, and is beneficial to solvation of sodium ions in electrolyte; adding a first additive vulcanization accelerator to enhance electrode surface film forming and to build a stable electrode/electrolyte interface; the nitrile material as the second additive is added to complex part of anions in the electrolyte, and the nitrile material and the solvation effect of the tetraethylene glycol dimethyl ether play a synergistic effect, so that the conductivity of the electrolyte is finally improved.
According to an embodiment of the present application, the base ether solvent is selected from at least one of tetrahydrofuran, 2-methyltetrahydrofuran, 1, 3-dioxolane, ethylene glycol dimethyl ether, dimethoxymethane, 1, 2-dimethoxyethane, diglyme, or diethoxyethane.
According to an embodiment of the application, the sodium salt is selected from the group consisting of NaPF 6 、NaBF 4 、NaClO 4 、Na(FSO 2 ) 2 N、Na (CF 3 SO 2 ) 2 N、Na (C 2 F 5 SO 2 ) 2 N、NaCF 3 SO 3 、NaAsF 6 、NaSbF 6 、NaBC 4 O 8 NaFSI, naTFSI, sodium salt of lower aliphatic carboxylic acid, naAlCl 4 、NaPO 2 F 2 Or Na (or) 2 PO 3 F.
According to an embodiment of the present application, the sodium salt is contained in an amount of 0.1wt.% to 10wt.%, based on 100% of the total mass of the electrolyte.
According to an embodiment of the application, the vulcanization accelerator is selected from at least one of CBC, N-tert-butyl-2-benzothiazole sulfenamide (TBBS), N-cyclohexyl-2-benzothiazole sulfenamide (CBS), N-tetramethyldithio-dicarboxamide (TMTD) or tetraethylthiuram disulfide (TETD), preferably TMTD and/or tetraethylthiuram disulfide (TETD).
According to an embodiment of the present application, the content of the vulcanization accelerator in the electrolyte is 0.1wt.% to 5wt.%, based on 100% of the total mass of the electrolyte.
According to an embodiment of the application, the nitrile material is selected from at least one of succinonitrile, glutaronitrile, adiponitrile, sebaconitrile, nondinitrile, dicyanobenzene or terephthalonitrile, preferably succinonitrile.
According to an embodiment of the present application, the nitrile material is contained in an amount of 1wt.% to 5wt.%, based on 100% of the total mass of the electrolyte.
According to an embodiment of the application, a third additive is further included in the electrolyte, the third additive being selected from ceramic powders. The addition of the third additive can widen the electrochemical window of the electrolyte and expand the selection range of the anode material.
Preferably, the ceramic powder comprises at least one of: siO (SiO) 2 Ceramic powder, beta' -Al 2 O 3 Ceramic powder, sodium super-ion conductor ceramic powder or sodium sulfide ion conductor ceramic powder.
According to the embodiment of the application, the content of the ceramic powder is 1-5 wt.% based on 100% of the total mass of the electrolyte.
The application also provides a preparation method of the electrolyte, which comprises the following steps:
s1: uniformly mixing a basic ether solvent and a long-chain ether solvent tetraethylene glycol dimethyl ether to obtain a mixed solvent;
s2: adding sodium salt into the mixed solvent in the step S1, and stirring until the mixed solvent is clear and transparent;
s3: adding the first additive, and stirring uniformly;
s4: and adding a second additive, optionally adding a third additive or not, and uniformly stirring to obtain the electrolyte.
According to an embodiment of the application, mixing means stirring. In the present application, the mixing time is not particularly limited as long as a uniform mixed solvent can be obtained, and for example, mixing means stirring for 2 hours. The stirring time is not particularly limited in the present application, as long as the additive is sufficiently dissolved in the mixed solvent, and for example, the stirring time is 2 hours, 4 hours or 24 hours.
The application also provides a sodium ion battery, which comprises the electrolyte.
According to the embodiment of the application, the sodium ion battery comprises the electrolyte, so that the sodium ion battery has the advantages of high charge and discharge efficiency, good cycle performance, high safety, wide working temperature range and low cost.
According to an embodiment of the present application, the sodium ion battery includes: the positive plate and the negative plate are provided with isolating films.
According to an embodiment of the present application, the positive electrode sheet includes, but is not limited to, at least one of the following sodium ion positive electrode active materials: transition metal oxides, prussian compounds, and polyanion compounds such as phosphates and fluorophosphates. Preferably, the sodium ion positive electrode active material is selected from sodium iron phosphate, sodium iron manganate, sodium titanium manganate or Na x MA[MB(CN) 6 ]·zH 2 At least one of O, wherein MA and MB are transition metal ions, independently selected from Fe 2+ 、Cu 2+ 、Cr 3+ Or Mn of 2+ X=0.1 to 4.0, and z=1 to 6.
According to an embodiment of the present application, the negative electrode sheet includes a metallic negative electrode material or a non-metallic negative electrode material.
Preferably, the metal anode material is selected from metal foils or alloy compounds including, but not limited to, metallic sodium, sodium alloys, tin, antimony, and the like.
Preferably, the nonmetallic anode material is selected from at least one of hard carbon, soft carbon, carbon nanotubes, expanded graphite, graphene and phosphorus.
According to an embodiment of the present application, the separator may be selected from any one of an insulating porous polymer film or an inorganic porous film, etc., which are conventionally used in the art, such as a porous polypropylene film, a porous polyethylene film, a porous composite polymer film, an insulating fiber paper, or a porous ceramic separator.
According to the embodiment of the application, the preparation method of the sodium ion battery is realized by adopting the technical scheme in the field.
Advantageous effects
The electrolyte is prepared by mixing basic ether electrolyte and long-chain ether solvent tetraethylene glycol dimethyl ether (TEGDME), and adding sodium salt, vulcanization accelerator, nitrile material and ceramic powder to obtain the sodium ion electrolyte with high electrochemistry and long cycle life. Has the following characteristics:
(1) The vulcanization accelerator in the sodium ion electrolyte has strong oxidation-reduction property, can promote the oxidation of the anode, and is beneficial to constructing a stable electrode electrolyte interface;
(2) The solvent TEGDME in the sodium ion electrolyte has high solvating capacity for free sodium ion salt, and is beneficial to solvating sodium ions in the electrolyte;
(3) The nitrile material and the vulcanization accelerator in the sodium ion electrolyte can complex part of anions, and the TEGDME is helpful for solvating sodium salt, and the additive is helpful for improving the conductivity of the electrolyte;
(4) The ceramic powder in the sodium ion electrolyte widens the electrochemical window of the electrolyte and enlarges the selection range of the anode material;
(5) The sodium ion electrolyte provided by the application has the advantages of simple preparation process, high yield and low cost, is suitable for industrial application, and has a wide application prospect in the fields of portable electronic equipment and power batteries.
Description of the embodiments
The technical scheme of the application will be further described in detail below with reference to specific embodiments. It is to be understood that the following examples are illustrative only and are not to be construed as limiting the scope of the application. All techniques implemented based on the above description of the application are intended to be included within the scope of the application.
Unless otherwise indicated, the starting materials and reagents used in the following examples were either commercially available or may be prepared by known methods.
The following is an abbreviation in the present application:
NaTFSI: sodium bis (trifluoromethyl) sulfonyl imide;
TETD: tetraethylthiuram disulfide;
SN: succinonitrile (succinonitrile);
DME: ethylene glycol dimethyl ether;
TEGDME: tetraethylene glycol dimethyl ether;
THF: tetrahydrofuran;
DMM: dipropylene glycol dimethyl ether;
TGM: triethylene glycol dimethyl ether;
g2, diethylene glycol dimethyl ether;
g3, triethylene glycol dimethyl ether;
g4, tetraethyleneglycol dimethyl ether.
Examples 1 to 26 and comparative examples 1 to 4
The sodium ion batteries of examples 1-26 and comparative examples 1-4 were prepared by the following method:
respectively preparing electrolyte according to the formula shown in table 1 to serve as electrolyte of the sodium ion battery;
na with specific capacity of 100mAh/g is adopted 2 Fe 2 (SO 4 ) 3 Is an anode active material, and is coated on an aluminum foil with PVDF and conductive carbon black according to the mass ratio of 95:3:2 to be used as an anode piece;
the negative plate is sodium metal; the membrane is a celgard 2400 polypropylene porous membrane;
and (3) sequentially overlapping and assembling the positive plate, the negative plate and the diaphragm, and then respectively adding the electrolyte to obtain the sodium ion battery, wherein the sodium ion battery is respectively marked as examples 1-26 and comparative examples 1-4.
The electrolytes of examples 1 to 20 all had the same solvent, except that the additives in the electrolytes were different:
the electrolytes of examples 1 to 5 were added with sodium salt alone;
the electrolytes of examples 6 to 10 were the same as in example 3 except that different kinds of vulcanization accelerators were added, respectively;
the electrolytes of examples 11 to 15 were the same as example 6 except that nitrile materials of different concentrations were added, respectively;
the electrolytes of examples 16 to 20 were the same as in example 14 except that ceramic powders of different concentrations were added respectively;
the electrolytes of examples 21 to 26 were the same as those of example 17 in the types and concentrations of additives, except that different solvent types were used in examples 21 to 26, respectively.
The electrolytes of comparative examples 1 to 4 were all known electrolytes, and specific components are shown in Table 1.
Test case
The sodium ion batteries of examples 1-26 and comparative examples 1-4 were respectively subjected to electrochemical performance testing as follows:
after the battery is assembled, a LAND blue battery testing system is used for testing the cycle performance under the conditions of 0.2C/0.2C charge-discharge current and 3.0V-4.4V charge-discharge voltage.
The test results are shown in Table 1.
Table 1 sodium ion battery performance test results
The electrolytes of examples 1 to 20 all had the same solvent, except that the additives in the electrolytes differed from each other as shown in table 1:
according to the test results of the embodiments 1-5, sodium salts with different concentrations are added into the electrolyte to improve the cycle performance of the battery to a certain extent, and the cycle performance is best when the NaTFSI content reaches 5%;
according to the test results of examples 6-10, after different types of vulcanization accelerators are respectively added when the sodium salt concentration is 5wt.%, the cyclic performance of the TETD test group of example 6 is further improved to 94.6%;
examples 11-15 are further added with nitrile materials with different concentrations based on example 6, wherein 4wt.% SN in example 14 gives better effect, and the cycle performance is further improved;
the electrolytes of examples 16 to 20 were different from example 14 in that ceramic powders were added at different concentrations, respectively, and from the test results of Table 1, 1.5wt.% NaZr was found 2 P 3 O 12 The ceramic addition amount of the ceramic is more obvious for improving the cycle performance, and the performance deterioration can occur when the ceramic is further added;
examples 21 to 26 the electrolyte of the example was the same as the additive of example 17 in the type and concentration, except that examples 21 to 26 each used a different solvent type, and it was found through verification that the effect of changing the different solvent type was not as good as that of example 17;
the electrolytes of comparative examples 1-4 all used known electrolytes, and the circulating effect was found to be far lower than in the optimized electrolyte examples of the present application;
according to the comparison, the sulfide accelerator and the nitrile material have further improving and optimizing effects on the electrolyte after the sodium salt is improved, and have better synergistic effect on improving the cycle performance of the battery.
The above description of exemplary embodiments of the application has been provided. However, the scope of the present application is not limited to the above embodiments. Any modifications, equivalent substitutions, improvements, or the like, which are within the spirit and principles of the present application, should be made by those skilled in the art, and are intended to be included within the scope of the present application.
Claims (5)
1. An electrolyte, characterized in that it comprises at least: a base ether solvent; long-chain ether solvent tetraethylene glycol dimethyl ether; a sodium salt; a first additive, a second additive, and a third additive; the first additive is a vulcanization accelerator; the second additive is a nitrile material; the third additive is selected from ceramic powder;
the vulcanization accelerator is at least one selected from N-tertiary butyl-2-benzothiazole sulfenamide, N-cyclohexyl-2-benzothiazole sulfenamide and N, N-tetramethyl disulfide dithio carbonyl amine;
the nitrile material is at least one selected from glutaronitrile, adiponitrile, sebaconitrile, nondinitrile, dicyanobenzene or terephthalonitrile;
the content of the vulcanization accelerator in the electrolyte is 0.1-5 wt%, the content of the nitrile material is 1-5 wt%, and the content of the ceramic powder is 1-5 wt%, based on 100% of the total mass of the electrolyte;
the ceramic powder comprises at least one of the following: sodium super ion conductor ceramic powder or sodium sulfide ion conductor ceramic powder;
the basic ether solvent is at least one selected from tetrahydrofuran, 2-methyltetrahydrofuran, 1, 3-dioxolane, ethylene glycol dimethyl ether, dimethoxymethane, 1, 2-dimethoxyethane, diethylene glycol dimethyl ether or diethoxyethane.
2. The electrolyte of claim 1 wherein the sodium salt is selected from the group consisting of NaPF 6 、NaBF 4 、NaClO 4 、Na(FSO 2 ) 2 N、Na (CF 3 SO 2 ) 2 N、Na (C 2 F 5 SO 2 ) 2 N、NaCF 3 SO 3 、NaAsF 6 、NaSbF 6 、NaBC 4 O 8 NaFSI, naTFSI, sodium salt of lower aliphatic carboxylic acid, naAlCl 4 、NaPO 2 F 2 Or Na (or) 2 PO 3 F.
3. The electrolyte according to claim 1, wherein the sodium salt is contained in an amount of 0.1wt.% to 10wt.%, based on 100% of the total mass of the electrolyte.
4. The electrolyte of claim 1 wherein the vulcanization accelerator is selected from the group consisting of N, N-tetramethyl dithiobis-thioamine.
5. A sodium ion battery, characterized in that it comprises the electrolyte according to any one of claims 1-4.
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| CN114400377B (en) * | 2021-12-28 | 2023-08-01 | 大连中比动力电池有限公司 | Additive and electrolyte for sodium ferrite sodium ion battery |
| CN116706237B (en) * | 2023-08-07 | 2023-12-15 | 浙江华宇钠电新能源科技有限公司 | Quick ion conductor additive, mixed electrolyte, sodium ion battery and vehicle |
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