CN114335720A - Electrolyte additive, electrolyte and sodium ion battery comprising electrolyte - Google Patents
Electrolyte additive, electrolyte and sodium ion battery comprising electrolyte Download PDFInfo
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- CN114335720A CN114335720A CN202111461688.XA CN202111461688A CN114335720A CN 114335720 A CN114335720 A CN 114335720A CN 202111461688 A CN202111461688 A CN 202111461688A CN 114335720 A CN114335720 A CN 114335720A
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Abstract
The invention belongs to the technical field of sodium ion batteries, and particularly relates to an electrolyte additive, electrolyte and a sodium ion battery comprising the electrolyte, wherein the electrolyte additive comprises an additive a and an additive b, and the additive a comprises one or more of a first compound shown as a formula I and a second compound shown as a formula II; wherein R1, R2, R3, R4, R5, R6, R7, R8 and R9 are respectively and independently selected from one of hydrogen, halogen atoms, alkyl or alkoxy groups with 1-10 carbon atoms, and alkanoyl or unsaturated alkyl groups with 2-10 carbon atoms, and H in the alkyl, unsaturated alkyl, alkoxy and alkanoyl groups can be partially or completely substituted by one or more of halogen atoms, cyano groups, carboxyl groups and sulfonic groups. The electrolyte additive is beneficial to improving the cycle performance and improving the high and low temperature capacity retention rate, the capacity recovery rate and the thickness expansion rate.
Description
Technical Field
The invention belongs to the technical field of sodium ion batteries, and particularly relates to an electrolyte additive, an electrolyte and a sodium ion battery comprising the electrolyte.
Background
Sodium is one of the elements with abundant reserves on the earth, has a working principle similar to that of a lithium ion battery, has the advantages of low cost, good safety, long-term large-scale storage and the like, and is more and more concerned by research and development personnel. However, the sodium ion battery has the defects of poor cycle performance, high-temperature storage and inflation, low first efficiency and the like, and the wide application of the sodium ion battery is restricted.
The electrolyte is one of the key materials of the sodium ion power battery, and has significant influence on the cycle, high-temperature and low-temperature performance and the like of the battery. In the three major components of the electrolyte, the formula of the lithium salt and the solvent is not changed greatly, and the additive is a key factor for improving the performance of the sodium-ion battery, so that the development of the additive and the electrolyte meeting the performance of the sodium-ion battery has important significance.
Disclosure of Invention
One of the objects of the present invention is: aiming at the defects of the prior art, the electrolyte additive is provided, so that the circulation performance of the electrolyte is effectively improved, and the high-low temperature capacity retention rate, the capacity recovery rate and the thickness expansion rate are improved.
In order to achieve the purpose, the invention adopts the following technical scheme:
an electrolyte additive comprises an additive a and an additive b, wherein the additive a comprises one or more of a first compound shown as a formula I and a second compound shown as a formula II;
wherein R1, R2, R3, R4, R5, R6, R7, R8 and R9 are respectively and independently selected from any one of hydrogen, a halogen atom, an alkyl group with 1-10 carbon atoms, an unsaturated alkyl group with 2-10 carbon atoms, an alkoxy group with 1-10 carbon atoms or an alkanoyl group with 2-10 carbon atoms, and H in the alkyl group, the unsaturated alkyl group, the alkoxy group and the alkanoyl group can be partially or completely substituted by one or more of a halogen atom, a cyano group, a carboxyl group and a sulfonic group; wherein the additive b is one or more of ethylene carbonate, fluoroethylene carbonate, ethylene carbonate, ethylene sulfate and propenyl sultone.
Preferably, in the first compound shown in the formula I, R1, R2 and R3 are halogen atoms, in the second compound shown in the formula II, R4, R5 and R6 are halogen atoms, and R7, R8 and R9 are alkyl groups with 1-10 carbon atoms.
Preferably, in the first compound, R1, R2 and R3 are fluorine, and in the second compound, R4, R5 and R6 are fluorine, and R7, R8 and R9 are methyl.
Preferably, the mass ratio of the additive a to the additive b is (1-5) to (1-5). The mass ratio of the additive a to the additive b is 1:1, 1:2, 1:3, 1:4, 1:5, 2:1, 3:1, 4:1 and 5: 1.
Preferably, the additive a is the first compound and the second compound, the mass ratio of the first compound to the second compound is 2:1, and the additive b is fluoroethylene carbonate.
The second purpose of the invention is: aiming at the defects of the prior art, the electrolyte is provided, and has excellent cycle performance and high and low temperature performance.
In order to achieve the purpose, the invention adopts the following technical scheme:
an electrolyte comprises a sodium salt electrolyte, an organic solvent and the electrolyte additive.
Preferably, the electrolyte additive accounts for 2-10% of the total mass of the electrolyte. The electrolyte additive accounts for 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9% and 10% of the total mass of the electrolyte.
Preferably, the organic solvent comprises a cyclic organic solvent and a chain organic solvent, the cyclic organic solvent is one or more of ethylene carbonate, propylene carbonate and butylene carbonate, and the chain organic solvent is one or more of dimethyl carbonate, diethyl carbonate and ethyl methyl carbonate.
Preferably, the sodium salt electrolyte is one or more of sodium hexafluorophosphate, sodium perchlorate, sodium tetrafluoroborate and sodium bifluoroxalato borate.
The third purpose of the invention is that: aiming at the defects of the prior art, the sodium ion battery has good cycle performance, high and low temperature performance, first efficiency, no flatulence during high-temperature storage and good safety.
In order to achieve the purpose, the invention adopts the following technical scheme:
a sodium ion battery comprises the electrolyte.
The sodium ion battery comprises a positive plate, a negative plate, a diaphragm, electrolyte and a shell. The positive electrode includes a current collector and an active material layer provided on the current collector. The active material layer includes but is not limited to the chemical formula of Na0.67MnxAyBzO2±δIn the molecular formula, A is one or more of Co, Ni and Cr, B is one or more of Mg, Al, Ca, Ti, Cu, Zn and Ba, and 0.6<x<1，0<y<0.1，0.6<x + y0, x + y + z is 1, 0 ≦ δ ≦ 0.1, and the positive electrode active material may also include, but is not limited to, Na1.845Mn[Fe(CN)6]0.961·1.988H2O、Na3V2(PO4)2O2F、Na3V1.95Mn0.05(PO4)2F3、Na3V1.95Mn0.05(PO4)2O2F、Na3V2(PO4)2F3And Na2.95Li0.05V2(PO4)2O2F, and the like. The positive electrode active material may be further modified, and the method of modifying the positive electrode active material is known to those skilled in the art, for example, the positive electrode active material may be modified by coating, doping, and the like, and the material used in the modification may be one or a combination of more of Al, B, P, Zr, Si, Ti, Ge, Sn, Mg, Ce, W, and the like, but is not limited thereto. And the positive electrode current collector is generally a structure or a part for collecting current, and the positive electrode current collector may be any material suitable for being used as a positive electrode current collector of a sodium ion battery in the field, for example, the positive electrode current collector may include, but is not limited to, a metal foil and the like, and more specifically, may include, but is not limited to, an aluminum foil and the like.
The negative electrode comprises a current collector and an active substance layer arranged on the surface of the current collector, wherein the active substance layer can be one or more of graphite, soft carbon, hard carbon, carbon fiber, mesocarbon microbeads, silicon-based materials, tin-based materials, lithium titanate or other metals capable of forming an alloy with sodium. Wherein, the graphite can be selected from one or more of artificial graphite, natural graphite and modified graphite; the silicon-based material can be one or more selected from simple substance silicon, silicon-oxygen compound, silicon-carbon compound and silicon alloy; the tin-based material can be one or more selected from simple substance tin, tin oxide compound and tin alloy. The negative electrode current collector is generally a structure or a part for collecting current, and may be any material suitable for use as a negative electrode current collector of a sodium ion battery in the art, for example, the negative electrode current collector may include, but is not limited to, a metal foil, and the like, and more specifically, may include, but is not limited to, a copper foil, and the like.
The separator may be any material suitable for a sodium ion battery separator in the art, and for example, may be a combination including, but not limited to, one or more of polyethylene, polypropylene, polyvinylidene fluoride, aramid, polyethylene terephthalate, polytetrafluoroethylene, polyacrylonitrile, polyimide, polyamide, polyester, natural fiber, and the like.
Compared with the prior art, the invention has the beneficial effects that: in the electrolyte additive, a first compound in the additive a is oxidized and decomposed at the positive electrode to form a stable CEI film, and the interface film contains B-O bonds, so that the electrolyte additive has higher ionic conductivity, reduces the internal resistance of a battery, reduces polarization, improves cycle performance, can improve the wettability of electrolyte and forms a more uniform low-impedance interface film; the second compound in the additive a, Si-O bond breaking can react with water and HF to prevent large-size water from enteringThe crystal lattice is extruded in the anode material, the stability of the material is improved, the hydrolysis of sodium salt can be inhibited, the stability of the electrolyte is improved, and the second compound has a fluorosulfonyl structure because of fluorine atoms and SO2And the fluorine-containing compound has good wettability and low film-forming impedance, and the performance of the battery is improved. The electrolyte additive can obviously improve the cycle and high-temperature storage performance of the battery, greatly reduces the gas production in the high-temperature storage process, and forms a more uniform and compact SEI film with small film impedance by being used in cooperation with the additive b, thereby further improving the cycle and high-temperature performance of the battery.
Detailed Description
The present invention will be described in further detail with reference to specific embodiments, but the embodiments of the present invention are not limited thereto.
Example 1
Preparing an electrolyte: mixing NaPF6Mixing organic solvent (EC (ethylene carbonate): DEC (diethyl carbonate): EMC (ethyl methyl carbonate): 3:2:5), additive a and additive b to obtain electrolyte, NaPF6The mass fractions of the organic solvent, the additive a and the additive b are 14%, 83%, 1% and 2%, respectively. The additive a is a mixture of a first compound and a second compound, wherein the mass ratio of the first compound to the second compound is 2:1, and the structures of the first compound and the second compound are as follows:
preparing a positive plate: the positive electrode material is Prussian blue positive electrode material Na1.72MnFe (CN)6, the positive electrode material, binder PVDF and conductive agent Super-P are dispersed in NMP organic solvent according to the mass ratio of 90:4:6, and are stirred to be stable and uniform under the action of a vacuum stirrer, and are uniformly coated on an aluminum foil with the thickness of 12 mu m. And (3) airing the aluminum foil at room temperature, transferring the aluminum foil to a blast oven at 120 ℃ for drying for 1h, and then performing cold pressing and die cutting to prepare the positive plate.
Preparing a negative plate: the spherical hard carbon, the PVDF binder and the Super-P conductive agent are mixed together according to the mass ratio of 97:2:1, and are dispersed in an NMP organic solvent, so that the spherical hard carbon, the PVDF binder and the Super-P conductive agent are uniformly coated on an aluminum foil with the thickness of 15 mu m. And (3) airing the aluminum foil at room temperature, transferring the aluminum foil to a blast oven at 120 ℃ for drying for 1h, and then performing cold pressing and die cutting to prepare the negative plate.
Preparing a sodium ion battery: and (2) obtaining a naked battery core by laminating the positive plate, the negative plate and the polypropylene ceramic diaphragm, filling the battery core into an aluminum-plastic film packaging shell, injecting the electrolyte, sequentially sealing, standing, performing hot-cold pressing, forming, grading and other processes, and thus obtaining the sodium ion battery.
Example 2
The difference from example 1 is that: the NaPF6The mass fractions of the organic solvent, the additive a and the additive b are 14%, 82%, 2% and 2%, respectively.
The rest is the same as embodiment 1, and the description is omitted here.
Example 3
The difference from example 1 is that: the NaPF6The mass fractions of the organic solvent, the additive a and the additive b are 14%, 79%, 5% and 2%, respectively.
The rest is the same as embodiment 1, and the description is omitted here.
Example 4
The difference from example 1 is that: the NaPF6The mass fractions of the organic solvent, the additive a and the additive b are 14%, 77%, 7% and 2%, respectively.
The rest is the same as embodiment 1, and the description is omitted here.
Example 5
The difference from example 1 is that: the additive a comprises a first compound and a second compound, and the structure is as follows:
the rest is the same as embodiment 1, and the description is omitted here.
Example 6
The difference from example 1 is that: the additive a comprises a first compound and a second compound, and the structure is as follows:
the rest is the same as embodiment 1, and the description is omitted here.
Example 7
The difference from example 1 is that: the additive a comprises a first compound and a second compound, and the structure is as follows:
the rest is the same as embodiment 1, and the description is omitted here.
Example 8
The difference from example 1 is that: additive a includes only the first compound, and the structure is as follows:
the rest is the same as embodiment 1, and the description is omitted here.
Example 9
The difference from example 1 is that: additive a includes only the second compound, and the structure is as follows:
the rest is the same as embodiment 1, and the description is omitted here.
Example 10
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 1: 1.
The rest is the same as embodiment 1, and the description is omitted here.
Example 11
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 3: 1.
The rest is the same as embodiment 1, and the description is omitted here.
Example 12
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 4: 1.
The rest is the same as embodiment 1, and the description is omitted here.
Example 13
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 5: 1.
The rest is the same as embodiment 1, and the description is omitted here.
Example 14
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 1: 2.
The rest is the same as embodiment 1, and the description is omitted here.
Example 15
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 1: 3.
The rest is the same as embodiment 1, and the description is omitted here.
Example 16
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 1: 4.
The rest is the same as embodiment 1, and the description is omitted here.
Example 17
The difference from example 1 is that: the mass ratio of the first compound to the second compound is 1: 5.
The rest is the same as embodiment 1, and the description is omitted here.
Comparative example 1
The difference from example 1 is that: NaPF6The mass fractions of the organic solvent and the additive b are 14%, 84% and 2%, respectively.
The rest is the same as embodiment 1, and the description is omitted here.
Comparative example 2
The difference from example 1 is that: NaPF6The mass fractions of the organic solvent and the additive a are 14%, 84% and 2%, respectively.
The rest is the same as embodiment 1, and the description is omitted here.
And (3) performance testing: the electrolyte additives prepared in the above examples 1 to 17 and comparative examples 1 and 2 were applied to an electrolyte and a sodium ion battery was prepared and tested, and the test results are reported in table 1.
TABLE 1
The performance of the electrolyte additive prepared by the invention is better than that of comparative example 1 and comparative example 2, the capacity retention rate of the electrolyte additive in 500 cycles at 55 ℃ reaches 94.3%, the capacity retention rate of the electrolyte additive in high-temperature storage at 60 ℃/7d reaches 97.1%, the capacity recovery rate is 99.8%, and the thickness expansion rate is 0.52%. From the comparison of examples 1-4, when the NaPF is set6And when the mass fractions of the organic solvent, the additive a and the additive b are 14%, 83%, 1% and 2%, respectively, the prepared electrolyte has better performance. From comparison of examples 1 and 5 to 9, when the additive a is set to have the following chemical formulas for the first compound and the second compound, respectively, the prepared electrolyte has better performance.
From comparison of examples 1 and 10 to 17, when the mass ratio of the first compound to the second compound is set to 2:1, the prepared electrolyte has better performance. From comparison of example 1 and comparative examples 1-2, the electrolyte prepared by using only additive a or only additive b has poor performance.
In conclusion, the sodium ion battery provided by the invention can effectively improve the cycle performance of the electrolyte and improve the high-low temperature capacity retention rate, the capacity recovery rate and the thickness expansion rate.
Variations and modifications to the above-described embodiments may also occur to those skilled in the art, which fall within the scope of the invention as disclosed and taught herein. Therefore, the present invention is not limited to the above-mentioned embodiments, and any obvious improvement, replacement or modification made by those skilled in the art based on the present invention is within the protection scope of the present invention. Furthermore, although specific terms are employed herein, they are used in a generic and descriptive sense only and not for purposes of limitation.
Claims (10)
1. An electrolyte additive is characterized by comprising an additive a and an additive b, wherein the additive a comprises one or more of a first compound shown as a formula I and a second compound shown as a formula II;
wherein R1, R2, R3, R4, R5, R6, R7, R8 and R9 are respectively and independently selected from any one of hydrogen, a halogen atom, an alkyl group with 1-10 carbon atoms, an unsaturated alkyl group with 2-10 carbon atoms, an alkoxy group with 1-10 carbon atoms or an alkanoyl group with 2-10 carbon atoms, and H in the alkyl group, the unsaturated alkyl group, the alkoxy group and the alkanoyl group can be partially or completely substituted by one or more of a halogen atom, a cyano group, a carboxyl group and a sulfonic group; wherein the additive b is one or more of ethylene carbonate, fluoroethylene carbonate, ethylene carbonate, ethylene sulfate and propenyl sultone.
2. The electrolyte additive as claimed in claim 1, wherein in the first compound represented by formula i, R1, R2 and R3 are halogen atoms, and in the second compound represented by formula ii, R4, R5 and R6 are halogen atoms, and R7, R8 and R9 are alkyl groups having 1 to 10 carbon atoms.
3. The electrolyte additive according to claim 1 or 2, wherein R1, R2, R3 are fluorine in the first compound, R4, R5, R6 are fluorine, and R7, R8, and R9 are methyl in the second compound.
4. The electrolyte additive as claimed in claim 1, wherein the mass ratio of the additive a to the additive b is (1-5): 1-5.
5. The electrolyte additive according to claim 1 or 4, wherein the additive a comprises the first compound and the second compound, the mass part ratio of the first compound to the second compound is 2:1, and the additive b is fluoroethylene carbonate.
6. An electrolyte comprising a sodium salt electrolyte, an organic solvent and the electrolyte additive of any one of claims 1 to 5.
7. The electrolyte of claim 6, wherein the electrolyte additive comprises 2% to 10% by mass of the total mass of the electrolyte.
8. The electrolyte of claim 6, wherein the organic solvent comprises a cyclic organic solvent and a chain organic solvent, the cyclic organic solvent is one or more of ethylene carbonate, propylene carbonate and butylene carbonate, and the chain organic solvent is one or more of dimethyl carbonate, diethyl carbonate and ethyl methyl carbonate.
9. The electrolyte of claim 6, wherein the sodium salt electrolyte is one or more of sodium hexafluorophosphate, sodium perchlorate, sodium tetrafluoroborate, and sodium bifluorodioxalato.
10. A sodium ion battery comprising the electrolyte of any one of claims 6 to 9.
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| CN202111461688.XA CN114335720A (en) | 2021-12-02 | 2021-12-02 | Electrolyte additive, electrolyte and sodium ion battery comprising electrolyte |
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| CN1409430A (en) * | 2001-09-20 | 2003-04-09 | 丰田自动车株式会社 | Secondary battery of non-water electrolyte |
| JP2004006237A (en) * | 2002-04-09 | 2004-01-08 | Toyota Motor Corp | Polymer electrolyte and polymer lithium battery |
| CN102035045A (en) * | 2009-09-24 | 2011-04-27 | 上海图尔实业发展有限公司 | Novel low-temperature flame-retardant electrolyte |
| US20150263386A1 (en) * | 2012-10-30 | 2015-09-17 | Basf Se | Lithium ion secondary battery comprising a silicon anode |
| CN111477955A (en) * | 2019-01-23 | 2020-07-31 | 现代自动车株式会社 | Electrolyte for lithium secondary battery and lithium secondary battery comprising the same |
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2021
- 2021-12-02 CN CN202111461688.XA patent/CN114335720A/en active Pending
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1409430A (en) * | 2001-09-20 | 2003-04-09 | 丰田自动车株式会社 | Secondary battery of non-water electrolyte |
| JP2004006237A (en) * | 2002-04-09 | 2004-01-08 | Toyota Motor Corp | Polymer electrolyte and polymer lithium battery |
| CN102035045A (en) * | 2009-09-24 | 2011-04-27 | 上海图尔实业发展有限公司 | Novel low-temperature flame-retardant electrolyte |
| US20150263386A1 (en) * | 2012-10-30 | 2015-09-17 | Basf Se | Lithium ion secondary battery comprising a silicon anode |
| CN111477955A (en) * | 2019-01-23 | 2020-07-31 | 现代自动车株式会社 | Electrolyte for lithium secondary battery and lithium secondary battery comprising the same |
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