CN114243114A - Additive and electrolyte for Prussian blue sodium ion battery - Google Patents
Additive and electrolyte for Prussian blue sodium ion battery Download PDFInfo
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- CN114243114A CN114243114A CN202111626276.7A CN202111626276A CN114243114A CN 114243114 A CN114243114 A CN 114243114A CN 202111626276 A CN202111626276 A CN 202111626276A CN 114243114 A CN114243114 A CN 114243114A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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Abstract
The invention relates to the field of batteries, in particular to an additive and electrolyte for a Prussian blue sodium ion battery. The additive comprises hexamethyldisilazane and imidazole containing a cyano group; wherein the mass percentage of the imidazole containing cyanogen groups in the additive for the electrolyte is 20-60%; the mass ratio of the hexamethyldisilazane to the imidazole containing the cyanogen group is (2-4): (1-3). The additive provided by the invention avoids adverse effects of water on substances in the electrolyte to a great extent, so that the circulation stability of the electrolyte is improved, and the circulation performance of the battery (especially including a Prussian blue type sodium ion battery) is greatly improved.
Description
Technical Field
The invention relates to the field of batteries, in particular to an additive and electrolyte for a Prussian blue sodium ion battery.
Background
In the 21 st century, lithium batteries are used in a variety of fields such as mobile phones, computers, wearable devices, electric automobiles, two-wheel bicycles, electric tools, street lamps and the like. With the increasing use amount of lithium batteries, the consumption amount of lithium resources shows a trend of increasing more and more. However, the increase in the production of lithium cannot be matched with the increase in the consumption of lithium because lithium resources are limited, mainly existing in the states of spodumene ores and salt lake lithium, and the salt lake lithium cannot be extracted in winter. The above situation has led to a trend in which the prices of lithium metal and compounds have risen in recent years.
In contrast, sodium is widely available and abundant, and the storage capacity is 420 times of that of lithium, and the price is far lower than that of lithium. With the rapid rising of the lithium price, the sodium ion battery is expected to be widely concerned with the cost which is 30 to 50 percent lower than that of the lithium ion battery, and particularly has attractive application prospect in the fields of energy storage, hybrid power and lead-acid battery replacement.
Currently, sodium ions can be classified as Na according to the positive electrode material3V2(PO4)3、NaFe1/3Ni1/3Mn1/3O3Prussian blue three batteries; compared with other two batteries, the Prussian blue battery has received more extensive attention and intensive research due to the fact that the Prussian blue battery does not contain precious metals and has higher gram capacity. However, it has been found that the cycle life of such cells is less than that of Na3V2(PO4)3、NaFe1/3Ni1/ 3Mn1/3O3A sodium-ion like battery.
The chemical formula of the Prussian blue is AxMc[M’(CN)6]1-y(b-H2O)6y·￡y·(i-H2O)zWherein A is alkali metal or alkaline earth metal cation, M, M 'is transition metal cation, which can be selected from one or more of Mn, Fe, Co, Ni, Cu, Zn, etc.. the £ is M' (CN)6Void, b-H2O is coordinated water, i-H2O is interstitial water, 0<x≤2，0<c≤1，0<y<1，0≤z≤16。
However, one common drawback with current prussian blue-based materials is their short cycle life.
Disclosure of Invention
The invention finds that a main reason for shortening the cycle life of the Prussian blue sodium ion battery is that in the charging and discharging processes, a part of void water and bound water of the anode material are separated from the anode, and can react with sodium hexafluorophosphate in electrolyte to generate hydrofluoric acid, and the generated hydrofluoric acid can accelerate the precipitation of alkali metals and alkaline earth metals in the Prussian blue material, catalyze the decomposition of an SEI (solid electrolyte interphase), and deteriorate the battery performance; resulting in irreversible sodium ion loss and thus poor battery cycling.
Therefore, the invention further explores and provides an additive and an electrolyte for the Prussian blue sodium-ion battery.
Specifically, the present invention firstly provides an additive for an electrolyte, which comprises: hexamethyldisilazane (HMDS) and imidazole containing cyano groups;
wherein the mass percentage of the imidazole containing cyanogen groups in the additive for the electrolyte is 20-60%; the mass ratio of the hexamethyldisilazane to the imidazole containing the cyanogen group is (2-4): (1-3).
The invention discovers that the electrolyte additive can avoid substances and H in the electrolyte to a greater extent2O reacts and thus the resulting loss of performance and life of the battery, such as that of a prussian blue-based sodium ion battery, can be avoided.
Preferably, the imidazole containing a cyano group is one or more selected from 2-fluoromethyl 4, 5-dicyanoimidazole, 4, 5-dicyano-2-trifluoromethyl-imidazole and 4, 5-dicyano-1-methyl-1H-imidazole.
Preferably, the mass percentage of the imidazole containing a cyano group in the additive for the electrolyte is 40-50%.
As a preferable scheme, the additive for the electrolyte consists of components in a mass ratio of 4: 6-8: 2 and imidazole containing a cyano group, more preferably in a mass ratio of 5: 5-6: 4.
further, the invention also provides an electrolyte, which contains the additive for the electrolyte.
Preferably, the mass percentage of the additive for the electrolyte in the electrolyte is 0.5-1.5%; more preferably 0.5 to 1%.
More preferably, the mass percentage of the imidazole containing cyanide groups in the electrolyte is 0.4-0.5%.
Preferably, the electrolyte further contains hexafluorophosphate, and the hexafluorophosphate is one or two of lithium hexafluorophosphate and sodium hexafluorophosphate.
The additive (especially HMDS) has good stabilizing effect on the substances in the electrolyte, and can avoid side reaction with impurities in the electrolyte.
Preferably, the electrolyte further contains sodium salt, and the sodium salt includes sodium hexafluorophosphate.
Sodium hexafluorophosphate is easy to generate hydrolysis reaction to generate hydrofluoric acid and damage a negative electrode SEI film, after the additive is added into electrolyte containing sodium hexafluorophosphate, cyano-group in an imidazole structure is complexed with water molecule through hydrogen bond to inhibit hydrolysis reaction, and hexamethyldisilazane can be further complexed with PF5Form hexa-ligand complex to reduce PF5Reduction of PF5And undergoes side reactions with impurities in the electrolyte, so that the battery performance can be significantly improved through dual effects.
Optionally, the sodium salt further comprises one or two of sodium perchlorate and sodium tetrafluoroborate.
Preferably, the mass percentage of the sodium salt in the electrolyte is 10-20%; preferably 15 to 20%.
Preferably, the electrolyte further contains an organic solvent, and the organic solvent comprises the following components in a mass ratio of (1-3): (5-8) a cyclic carbonate and a chain carbonate;
wherein the cyclic carbonate is selected from one or two of ethylene carbonate and propylene carbonate;
the chain carbonate is selected from one or more of dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, dipropyl carbonate and methyl propyl carbonate.
As a preferred embodiment, the electrolyte of the present invention contains the following components in parts by weight: 79-89.5 parts of organic solvent, 10-20 parts of sodium salt and 0.5-1 part of additive for electrolyte.
Furthermore, the invention also provides a battery containing the electrolyte.
Preferably, the positive electrode material of the battery contains interstitial water and/or bound water. In this case, water in the positive electrode material is liable to adversely affect the substances in the electrolyte, and hence a greater degree of improvement in performance can be obtained when the additive for an electrolyte or the electrolyte of the present invention is applied.
More preferably, the positive electrode material of the battery contains a prussian blue material. The void water and the bound water of the material are separated from the anode and cause negative influence on the electrolyte performance, and the performance can be improved to a great extent when the additive or the electrolyte for the electrolyte is applied.
In a preferred embodiment, the positive electrode material of the battery contains a prussian blue material, and the electrolyte contains sodium hexafluorophosphate and the additive for an electrolyte solution of the present invention.
Based on the technical scheme, the invention has the beneficial effects that:
the additive provided by the invention avoids adverse effects of water on substances in the electrolyte to a great extent, so that the circulation stability of the electrolyte is improved, and the circulation performance of the battery (especially including a Prussian blue type sodium ion battery) is greatly improved.
Detailed Description
The following examples are intended to illustrate the invention but are not intended to limit the scope of the invention.
In order to more favorably compare the effects of the additives, the same sodium salt and organic solvent are used in the electrolytes of the following examples, and in fact, the effects of the present invention are exhibited as long as the sodium salt and organic solvent used are within the range defined by the present invention.
The examples do not show the specific techniques or conditions, according to the technical or conditions described in the literature in the field, or according to the product specifications. The reagents or instruments used are conventional products available from regular distributors, not indicated by the manufacturer.
Example 1
The present example provides an additive for an electrolyte, which contains, by mass, 4: 1 hexamethyldisilazane and 2-fluoromethyl 4, 5-dicyanoimidazole.
This example further provides an electrolyte containing the above additive, and the formulation thereof is as follows: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate, 0.2g of 2-fluoromethyl 4, 5-dicyanoimidazole and 0.8g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Example 2
The present example provides an additive for an electrolyte, which contains, by mass, 4: 1 hexamethyldisilazane and 4, 5-dicyano-2-trifluoromethyl-imidazole.
This example further provides an electrolyte containing the above additive, and the formulation thereof is as follows: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate, 0.2g of 4, 5-dicyano-2-trifluoromethyl-imidazole and 0.8g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Example 3
The present example provides an additive for an electrolyte, which contains, by mass, 4: 1 hexamethyldisilazane and 4, 5-dicyano-1-methyl-1H-imidazole.
This example further provides an electrolyte containing the above additive, and the formulation thereof is as follows: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate, 0.2g of 4, 5-dicyano-1-methyl-1H-imidazole and 0.8g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Example 4
The present example provides an additive for an electrolyte, which contains, by mass, 7: 3 hexamethyldisilazane and 2-fluoromethyl 4, 5-dicyanoimidazole.
This example further provides an electrolyte containing the above additive, and the formulation thereof is as follows: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate, 0.3g of 2-fluoromethyl 4, 5-dicyanoimidazole and 0.7g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Example 5
The present embodiment provides an additive for an electrolyte, which contains, by mass, 3: 2 hexamethyldisilazane and 2-fluoromethyl 4, 5-dicyanoimidazole.
This example further provides an electrolyte containing the above additive, and the formulation thereof is as follows: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate, 0.4g of 2-fluoromethyl 4, 5-dicyanoimidazole and 0.6g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Example 6
The present example provides an additive for an electrolyte, which contains, by mass, 1: 1 hexamethyldisilazane and 2-fluoromethyl 4, 5-dicyanoimidazole.
This example further provides an electrolyte containing the above additive, and the formulation thereof is as follows: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate, 0.5g of 2-fluoromethyl 4, 5-dicyanoimidazole and 0.5g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Example 7
The present embodiment provides an additive for an electrolyte, which contains, by mass, 2: 3 hexamethyldisilazane and 2-fluoromethyl 4, 5-dicyanoimidazole.
This example further provides an electrolyte containing the above additive, and the formulation thereof is as follows: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate, 0.6g of 2-fluoromethyl 4, 5-dicyanoimidazole and 0.4g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Comparative example 1
The comparative example provides an electrolyte having the following formulation: 18.18g of sodium hexafluorophosphate, 31.31g of ethylene carbonate, 25.25g of dimethyl carbonate and 25.25g of methyl ethyl carbonate.
The preparation method comprises mixing the above materials.
Comparative example 2
The comparative example provides an electrolyte having the following formulation: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate and 1g of 2-fluoromethyl 4, 5-dicyanoimidazole.
The preparation method comprises mixing the above materials.
Comparative example 3
The comparative example provides an electrolyte having the following formulation: 18g of sodium hexafluorophosphate, 31g of ethylene carbonate, 25g of dimethyl carbonate, 25g of methyl ethyl carbonate and 1g of hexamethyldisilazane.
The preparation method comprises mixing the above materials.
Comparative example 4
This comparative example provides an electrolyte which differs from example 6 only in that: replacement of 2-fluoromethyl 4, 5-dicyanoimidazole with an equal amount of LiB (C)2O4)(CN)2。
Examples of the experiments
The electrolytes of the examples and the comparative examples were injected into 26650 to 2.8Ah sodium ion battery cells (positive electrode prussian blue, negative electrode hard carbon) to prepare batteries.
And (3) carrying out cycle test on the prepared battery, cycling for 500 times, recording the discharge capacity of the battery at the first time and the 500 th time, and calculating the discharge retention rate. The calculation formula is as follows: the discharge retention rate was 100% of the first discharge capacity/500 th discharge capacity. The results are shown in Table 1.
TABLE 1
In comparison with examples 1-3, the three cyanogen-containing imidazole additives have basically consistent effects on the cycle life of the sodium ion battery. Meanwhile, the cycle life of the embodiment of the invention is obviously better than that of the comparative example.
In comparison with examples 1 and 4 to 7, the addition amount of the cyanogen-containing imidazole is in the range of 0.4 to 0.5%, and the sodium ion battery has the optimal cycle life.
Although the invention has been described in detail hereinabove with respect to a general description and specific embodiments thereof, it will be apparent to those skilled in the art that modifications or improvements may be made thereto based on the invention. Accordingly, such modifications and improvements are intended to be within the scope of the invention as claimed.
Claims (10)
1. An additive for an electrolyte, characterized by comprising: hexamethyldisilazane and imidazole containing a cyano group;
wherein the mass percentage of the imidazole containing cyanogen groups in the additive for the electrolyte is 20-60%; the mass ratio of the hexamethyldisilazane to the imidazole containing the cyanogen group is (2-4): (1-3).
2. The additive for electrolytic solutions according to claim 1, wherein the imidazole containing a cyano group is one or more selected from the group consisting of 2-fluoromethyl 4, 5-dicyanoimidazole, 4, 5-dicyano-2-trifluoromethyl-imidazole and 4, 5-dicyano-1-methyl-1H-imidazole.
3. The additive for an electrolyte solution according to claim 1 or 2, wherein the imidazole containing a cyano group is contained in the additive for an electrolyte solution in an amount of 40 to 50% by mass.
4. An electrolyte solution, characterized by comprising the additive for electrolyte solutions according to any one of claims 1 to 3.
5. The electrolyte according to claim 4, wherein the additive for the electrolyte is 0.5 to 1.5% by mass of the electrolyte; preferably 0.5 to 1%.
6. The electrolyte according to claim 4 or 5, further comprising a hexafluorophosphate salt selected from one or both of lithium hexafluorophosphate and sodium hexafluorophosphate.
7. The electrolyte of claim 4 or 5, further comprising sodium salts, including sodium hexafluorophosphate; optionally, the sodium salt further comprises one or two of sodium perchlorate and sodium tetrafluoroborate;
preferably, the mass percentage of the sodium salt in the electrolyte is 10-20%; preferably 15 to 20%.
8. The electrolyte according to any one of claims 4 to 7, further comprising an organic solvent, wherein the organic solvent comprises the following components in a mass ratio of (1-3): (5-8) a cyclic carbonate and a chain carbonate;
wherein the cyclic carbonate is selected from one or two of ethylene carbonate and propylene carbonate;
the chain carbonate is selected from one or more of dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, dipropyl carbonate and methyl propyl carbonate.
9. A battery comprising the electrolyte according to any one of claims 4 to 8.
10. The battery according to claim 9, wherein the positive electrode material contains interstitial water and/or bound water, and preferably the positive electrode material contains a prussian blue material.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
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| CN202111626276.7A CN114243114A (en) | 2021-12-28 | 2021-12-28 | Additive and electrolyte for Prussian blue sodium ion battery |
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| Application Number | Priority Date | Filing Date | Title |
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| CN202111626276.7A CN114243114A (en) | 2021-12-28 | 2021-12-28 | Additive and electrolyte for Prussian blue sodium ion battery |
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Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
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| US20150200422A1 (en) * | 2014-01-16 | 2015-07-16 | Samsung Sdi Co., Ltd. | Electrolyte additive for lithium battery, electrolyte including the same, and lithium battery including the electrolyte |
| US20160020488A1 (en) * | 2014-07-16 | 2016-01-21 | Samsung Sdi Co., Ltd. | Electrolyte additive for lithium battery, electrolyte including the additive, and lithium battery including the electrolyte |
| US20160351963A1 (en) * | 2015-06-01 | 2016-12-01 | Samsung Sdi Co., Ltd. | Electrolyte additive for lithium battery, electrolyte for lithium battery, and lithium battery including the electrolyte additive |
| CN110061291A (en) * | 2019-03-26 | 2019-07-26 | 天津市捷威动力工业有限公司 | A kind of high-temperature stable electrolyte and its lithium ion battery |
| CN111082140A (en) * | 2019-12-19 | 2020-04-28 | 东莞市坤乾新能源科技有限公司 | Novel sodium ion battery electrolyte and sodium battery |
| CN111261938A (en) * | 2018-11-30 | 2020-06-09 | 哈尔滨工业大学 | Electrolyte additive for sodium ion battery using prussian blue and analogues thereof as positive electrode material and application of electrolyte additive |
| CN111710906A (en) * | 2019-11-28 | 2020-09-25 | 湖北九邦新能源科技有限公司 | High-stability lithium ion battery electrolyte and battery containing same |
-
2021
- 2021-12-28 CN CN202111626276.7A patent/CN114243114A/en active Pending
Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20150200422A1 (en) * | 2014-01-16 | 2015-07-16 | Samsung Sdi Co., Ltd. | Electrolyte additive for lithium battery, electrolyte including the same, and lithium battery including the electrolyte |
| US20160020488A1 (en) * | 2014-07-16 | 2016-01-21 | Samsung Sdi Co., Ltd. | Electrolyte additive for lithium battery, electrolyte including the additive, and lithium battery including the electrolyte |
| US20160351963A1 (en) * | 2015-06-01 | 2016-12-01 | Samsung Sdi Co., Ltd. | Electrolyte additive for lithium battery, electrolyte for lithium battery, and lithium battery including the electrolyte additive |
| CN111261938A (en) * | 2018-11-30 | 2020-06-09 | 哈尔滨工业大学 | Electrolyte additive for sodium ion battery using prussian blue and analogues thereof as positive electrode material and application of electrolyte additive |
| CN110061291A (en) * | 2019-03-26 | 2019-07-26 | 天津市捷威动力工业有限公司 | A kind of high-temperature stable electrolyte and its lithium ion battery |
| CN111710906A (en) * | 2019-11-28 | 2020-09-25 | 湖北九邦新能源科技有限公司 | High-stability lithium ion battery electrolyte and battery containing same |
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