CN106910934A - A kind of silicon-based anode lithium-ion battery electrolytes - Google Patents
A kind of silicon-based anode lithium-ion battery electrolytes Download PDFInfo
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- CN106910934A CN106910934A CN201710078656.9A CN201710078656A CN106910934A CN 106910934 A CN106910934 A CN 106910934A CN 201710078656 A CN201710078656 A CN 201710078656A CN 106910934 A CN106910934 A CN 106910934A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- 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
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Abstract
The present invention provides a kind of silicon-based anode lithium-ion battery electrolytes, including organic solvent, lithium salts, film for additive and functional additive；The film for additive includes fluoro carbonic ester and three (pentafluorophenyl group) borines and the fluoro carbonic ester and the addition of described three (pentafluorophenyl group) borines are respectively 1% the 15% and 0.1% 5% of the electrolyte gross mass.The invention forms the SEI films of stabilization, uniform, flexible on silicon-based anode surface, the volumetric expansion that silicon-based anode is produced during repeated charge can be born, so as to lift the cycle performance of battery.
Description
【Technical field】
The invention belongs to technical field of lithium ion, more particularly to a kind of silicon-based anode lithium-ion battery electrolytes.
【Background technology】
, used as current gram volume highest lithium ion battery negative material, volume is significantly during removal lithium embedded for silica-base material
Degree expansion makes negative pole produce a large amount of micro-cracks with the stress that brings is shunk, and causes between active material, active material and collector
Between loose contact, so as to cause active material peel off and structural breakdown, cause electric conductivity reduction, the internal resistance of cell increase, therefore
Silicon-based anode lithium ion battery has that coulombic efficiency is low, high rate performance is poor, cycle life first.
The lifting of performance of lithium ion battery relies on the mutual cooperation of positive pole, negative pole, barrier film and electrolyte, can by with silicon
The electrolyte that base negative pole matches improves the performance of lithium ion battery, and Normal practice is to add film for additive in the electrolytic solution,
Such as FEC (fluorinated ethylene carbonate), VC (addition vinylene carbonate).FEC can form uniform, stabilization in negative terminal surface
SEI (Solid Electrolyte Interface) film, but temperature tolerance is poor, is easily decomposed under high temperature；And if FEC additions not
Foot, also results in circulation later stage performance degradation.VC is thicker in the SEI films that negative terminal surface is formed, and film forming procedure consumption is more
Lithium and film for additive, cause the coulombic efficiency first of battery relatively low, and the blocked up battery impedance that also results in of film forming increases, influence times
Rate performance.
In consideration of it, real be necessary to provide a kind of silicon-based anode lithium-ion battery electrolytes to overcome disadvantages described above.
【The content of the invention】
The present invention provides one kind can improve cathode film formation performance, and improve the silicon-based anode of cycle performance and high-temperature behavior
Lithium-ion battery electrolytes.
A kind of silicon-based anode lithium-ion battery electrolytes that the present invention is provided, including organic solvent, lithium salts, film for additive
And functional additive；The film for additive include fluoro carbonic ester and three (pentafluorophenyl group) borines and the fluoro carbonic ester with
The addition of described three (pentafluorophenyl group) borine is respectively the 1%-15% and 0.1%-5% of the electrolyte gross mass.
In a preferred embodiment, the organic solvent is cyclic carbonate or linear carbonate.
In a preferred embodiment, the organic solvent be ethylene carbonate, propene carbonate, methyl ethyl carbonate,
At least one in dimethyl carbonate, diethyl carbonate, ethyl acetate, propyl acetate, methyl propionate and ethyl propionate.
In a preferred embodiment, the lithium salts is lithium hexafluoro phosphate, LiBF4, hexafluoroarsenate lithium, difluoro
In Lithium bis (oxalate) borate, trimethyl fluoride sulfonyl lithium, double (fluorine sulphonyl) imine lithiums and double (trimethyl fluoride sulfonyl) imine lithiums at least one
Kind.
In a preferred embodiment, molar concentration of the lithium salts in the electrolyte is 0.3mol/L-1.5mo
l/L。
In a preferred embodiment, the fluoro carbonic ester be fluorinated ethylene carbonate, difluorinated ethylene carbonate,
Three fluoropropylene carbonates or two fluoropropylene carbonates.
In a preferred embodiment, the functional additive be (fluorine sulphonyl) (positive perfluoro butyl sulphonyl) imine lithium,
Difluoro lithium sulfimide, double (trifluoromethyl sulfonyl) imide lis, double (pentafluoroethyl group sulfonyl) imide lis, difluoro first
The double sulfimide lithiums of basic ring di-sulfonyl imides lithium, four fluoro ethyl rings or the double sulfimide lithiums of hexafluoro propyl group ring.
In a preferred embodiment, the addition of the functional additive is the 0.1%- of the electrolyte gross mass
5%.
In the silicon-based anode lithium-ion battery electrolytes that the present invention is provided, by fluoro carbonic ester and three (pentafluorophenyl group) borines
Be used in combination as film for additive, with more preferable film forming function, can silicon-based anode surface formed stabilization, it is uniform, have
The SEI films of toughness；Three (pentafluorophenyl group) borines connection can lift LiF solubility in the electrolytic solution, reduce the LiF in SEI films
Content, is conducive to lifting the stability of SEI films and reducing its impedance；Additionally, fluoro sulfimide class salt is used as functional additive
Fluorine ion can be rapidly discharged on silicon-based anode surface and form high-quality lithium fluoride film, be conducive to the transmission of lithium ion.Therefore,
The SEI films for being formed can bear the volumetric expansion that silicon-based anode is produced during repeated charge, so as to lift cyclicity
Energy.
【Brief description of the drawings】
Button cells of the Fig. 1 for the silicon-based anode lithium-ion battery electrolytes for providing of the invention in various embodiments is followed
Ring performance test curve comparison figure.
【Specific embodiment】
In order that the purpose of the present invention, technical scheme and Advantageous Effects become apparent from understanding, below in conjunction with accompanying drawing and
Specific embodiment, the present invention will be described in further detail.It should be appreciated that the specific implementation described in this specification
Mode is not intended to limit the present invention just for the sake of explaining the present invention.
The present invention provides a kind of silicon-based anode lithium-ion battery electrolytes, including organic solvent, lithium salts, film for additive and
Functional additive.
Specifically, the organic solvent is cyclic carbonate or linear carbonate.Preferably, the organic solvent is carbonic acid
Vinyl acetate, propene carbonate, methyl ethyl carbonate, dimethyl carbonate, diethyl carbonate, ethyl acetate, propyl acetate, methyl propionate
And at least one in ethyl propionate.
The lithium salts is lithium hexafluoro phosphate, LiBF4, hexafluoroarsenate lithium, difluorine oxalic acid boracic acid lithium, trifluoromethyl sulphur
At least one in acyl lithium, double (fluorine sulphonyl) imine lithiums and double (trimethyl fluoride sulfonyl) imine lithiums.Further, the lithium salts exists
Molar concentration in the electrolyte is 0.3mol/L-1.5mol/L.
The film for additive include fluoro carbonic ester and three (pentafluorophenyl group) borines and the fluoro carbonic ester with it is described
The addition of three (pentafluorophenyl group) borines is respectively the 1%-15% and 0.1%-5% of the electrolyte gross mass.The fluoro
Carbonic ester is fluorinated ethylene carbonate, difluorinated ethylene carbonate, three fluoropropylene carbonates or two fluoropropylene carbonates.
The functional additive is (fluorine sulphonyl) (positive perfluoro butyl sulphonyl) imine lithium, difluoro lithium sulfimide, double (three
Methyl fluoride sulfonyl) imide li, double (pentafluoroethyl group sulfonyl) imide lis, difluoromethyl ring di-sulfonyl imides lithium, tetrafluoro
The double sulfimide lithiums of ethyl ring or the double sulfimide lithiums of hexafluoro propyl group ring.Further, the addition of the functional additive is
The 0.1%-5% of the electrolyte gross mass.
Comparative example
At room temperature, in the glove box full of argon gas, ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate are pressed first
According to quality 1:1:1 quality is than organic solvent described in mixed configuration；Fluorinated ethylene carbonate is subsequently adding as film for additive,
And the addition of the fluorinated ethylene carbonate is the 5% of the organic solvent quality；Lithium hexafluoro phosphate is eventually adding as lithium
Salt, and molar concentration of the lithium hexafluoro phosphate in the electrolyte is 1.0mol/L.
Embodiment 1
At room temperature, in the glove box full of argon gas, ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate are pressed first
According to quality 1:1:1 quality is than organic solvent described in mixed configuration；It is subsequently adding fluorinated ethylene carbonate and three (pentafluorophenyl groups)
Borine is used as film for additive, and the fluorinated ethylene carbonate and the addition of described three (pentafluorophenyl group) borines are respectively institutes
State 5%, the 1% of organic solvent quality；Lithium hexafluoro phosphate is subsequently adding as lithium salts, and the lithium hexafluoro phosphate is in the electrolysis
Molar concentration in liquid is 1.0mol/L；Difluoro lithium sulfimide is eventually adding as functional additive, and described pair of fluoro
Sulfimide lithium is the 0.5% of the organic solvent quality.
Embodiment 2
At room temperature, in the glove box full of argon gas, ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate are pressed first
According to quality 1:1:1 quality is than organic solvent described in mixed configuration；It is subsequently adding fluorinated ethylene carbonate and three (pentafluorophenyl groups)
Borine is used as film for additive, and the fluorinated ethylene carbonate and the addition of described three (pentafluorophenyl group) borines are respectively institutes
State 5%, the 2% of organic solvent quality；Lithium hexafluoro phosphate is subsequently adding as lithium salts, and the lithium hexafluoro phosphate is in the electrolysis
Molar concentration in liquid is 1.0mol/L；Difluoro lithium sulfimide is eventually adding as functional additive, and described pair of fluoro
Sulfimide lithium is the 0.5% of the organic solvent quality.
Embodiment 3
At room temperature, in the glove box full of argon gas, ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate are pressed first
According to quality 1:1:1 quality is than organic solvent described in mixed configuration；It is subsequently adding fluorinated ethylene carbonate and three (pentafluorophenyl groups)
Borine is used as film for additive, and the fluorinated ethylene carbonate and the addition of described three (pentafluorophenyl group) borines are respectively institutes
State 5%, the 4% of organic solvent quality；Lithium hexafluoro phosphate is subsequently adding as lithium salts, and the lithium hexafluoro phosphate is in the electrolysis
Molar concentration in liquid is 1.0mol/L；Difluoro lithium sulfimide is eventually adding as functional additive, and described pair of fluoro
Sulfimide lithium is the 0.5% of the organic solvent quality.
Embodiment 4
At room temperature, in the glove box full of argon gas, ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate are pressed first
According to quality 1:1:1 quality is than organic solvent described in mixed configuration；It is subsequently adding fluorinated ethylene carbonate and three (pentafluorophenyl groups)
Borine is used as film for additive, and the fluorinated ethylene carbonate and the addition of described three (pentafluorophenyl group) borines are respectively institutes
State 5%, the 4% of organic solvent quality；Lithium hexafluoro phosphate is subsequently adding as lithium salts, and the lithium hexafluoro phosphate is in the electrolysis
Molar concentration in liquid is 1.0mol/L；Difluoro lithium sulfimide is eventually adding as functional additive, and described pair of fluoro
Sulfimide lithium is the 2% of the organic solvent quality.
By embodiment 1, embodiment 2, embodiment 3, embodiment 4 and comparative example respectively with LiFePO4, barrier film PE and silicon substrate
Negative pole is assembled into CR2023 button cells, carries out the constant current charge-discharge loop test that normal temperature 1C circulates 300 weeks, wherein, voltage
Scope is 3.65-2.00V；And in the environment of 60 DEG C it is aging shelve 10 days after measure capability retention and capacity restoration rate.
Fig. 1 is refer to, the electrolyte obtained by embodiment 1, embodiment 2, embodiment 3, embodiment 4 and comparative example is made button
Formula battery simultaneously carries out the result of charge and discharge cycles test and shows：Fluoro carbonic ester is with three (pentafluorophenyl group) borines in silicon-based anode lithium
It is used in combination as film for additive in ion electrolyte, the cycle performance of the button cell for obtaining is improved, wherein, with
During embodiment 4 is for the button cell charge and discharge cycles test of electrolyte, capability retention is 94.34%, cycle performance after 300 weeks
Larger lifting is obtained.
| Group | Comparative example | Embodiment 1 | Embodiment 2 | Embodiment 3 | Embodiment 4 |
| Capability retention | 76.23% | 80.68% | 81.81% | 82.56% | 84.35% |
| Capacity restoration rate | 80.50% | 83.11% | 84.54% | 86.85% | 88.24% |
As shown above, the electrolyte for being obtained by embodiment 1, embodiment 2, embodiment 3, embodiment 4 and comparative example is made
Button cell it is aging after measurement result show：With the addition of the button of fluoro carbonic ester and the electrolyte of three (pentafluorophenyl group) borines
The capability retention and capacity restoration rate of formula battery are obtained for improvement, illustrate that high temperature ageing performance has obtained larger lifting.
In the silicon-based anode lithium-ion battery electrolytes that the present invention is provided, by fluoro carbonic ester and three (pentafluorophenyl group) borines
Be used in combination as film for additive, with more preferable film forming function, can silicon-based anode surface formed stabilization, it is uniform, have
The SEI films of toughness；Three (pentafluorophenyl group) borines connection can lift LiF solubility in the electrolytic solution, reduce the LiF in SEI films
Content, is conducive to lifting the stability of SEI films and reducing its impedance；Additionally, fluoro sulfimide class salt is used as functional additive
Fluorine ion can be rapidly discharged on silicon-based anode surface and form high-quality lithium fluoride film, be conducive to the transmission of lithium ion.Therefore,
The SEI films for being formed can bear the volumetric expansion that silicon-based anode is produced during repeated charge, so as to lift cyclicity
Energy.
Presently preferred embodiments of the present invention is the foregoing is only, is to combine specific preferred embodiment to institute of the present invention
The further description of work, it is impossible to assert that specific implementation of the invention is confined to these explanations.It is all it is of the invention spirit and
Any modification, equivalent and improvement for being made within principle etc., should be included within the scope of the present invention.
Claims (8)
1. a kind of silicon-based anode lithium-ion battery electrolytes, it is characterised in that：Including organic solvent, lithium salts, film for additive and
Functional additive；The film for additive includes fluoro carbonic ester and three (pentafluorophenyl group) borines and the fluoro carbonic ester and institute
The addition for stating three (pentafluorophenyl group) borines is respectively the 1%-15% and 0.1%-5% of the electrolyte gross mass.
2. silicon-based anode lithium-ion battery electrolytes as claimed in claim 1, it is characterised in that：The organic solvent is ring-type
Carbonic ester or linear carbonate.
3. silicon-based anode lithium-ion battery electrolytes as claimed in claim 2, it is characterised in that：The organic solvent is carbonic acid
Vinyl acetate, propene carbonate, methyl ethyl carbonate, dimethyl carbonate, diethyl carbonate, ethyl acetate, propyl acetate, methyl propionate
And at least one in ethyl propionate.
4. silicon-based anode lithium-ion battery electrolytes as claimed in claim 1, it is characterised in that：The lithium salts is hexafluorophosphoric acid
Lithium, LiBF4, hexafluoroarsenate lithium, difluorine oxalic acid boracic acid lithium, trimethyl fluoride sulfonyl lithium, double (fluorine sulphonyl) imine lithiums and double
At least one in (trimethyl fluoride sulfonyl) imine lithium.
5. silicon-based anode lithium-ion battery electrolytes as claimed in claim 4, it is characterised in that：The lithium salts is in the electrolysis
Molar concentration in liquid is 0.3mol/L-1.5mol/L.
6. silicon-based anode lithium-ion battery electrolytes as claimed in claim 1, it is characterised in that：The fluoro carbonic ester is fluorine
For ethylene carbonate, difluorinated ethylene carbonate, three fluoropropylene carbonates or two fluoropropylene carbonates.
7. silicon-based anode lithium-ion battery electrolytes as claimed in claim 1, it is characterised in that：The functional additive is
It is (fluorine sulphonyl) (positive perfluoro butyl sulphonyl) imine lithium, difluoro lithium sulfimide, double (trifluoromethyl sulfonyl) imide lis, double
The double sulfimide lithiums of (pentafluoroethyl group sulfonyl) imide li, difluoromethyl ring di-sulfonyl imides lithium, four fluoro ethyl rings or hexafluoro
The double sulfimide lithiums of propyl group ring.
8. silicon-based anode lithium-ion battery electrolytes as claimed in claim 7, it is characterised in that：The functional additive adds
Dosage is the 0.1%-5% of the electrolyte gross mass.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109088099A (en) * | 2018-06-28 | 2018-12-25 | 华南师范大学 | A kind of sulphonyl class electrolysis additive for taking into account high temperature performance and the electrolyte containing the additive |
| CN109802179A (en) * | 2019-01-03 | 2019-05-24 | 东莞市杉杉电池材料有限公司 | A kind of high-energy density ferrous phosphate lithium battery electrolyte and lithium ion battery |
| CN111276675A (en) * | 2018-12-04 | 2020-06-12 | 中国科学院宁波材料技术与工程研究所 | Modified silicon-carbon material and preparation method and application thereof |
| CN112467222A (en) * | 2020-10-23 | 2021-03-09 | 福建南平延平区南孚新能源科技有限公司 | Button secondary battery |
| CN113823841A (en) * | 2021-10-29 | 2021-12-21 | 湖南法恩莱特新能源科技有限公司 | Electrolyte and preparation method and application thereof |
-
2017
- 2017-02-14 CN CN201710078656.9A patent/CN106910934A/en active Pending
Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109088099A (en) * | 2018-06-28 | 2018-12-25 | 华南师范大学 | A kind of sulphonyl class electrolysis additive for taking into account high temperature performance and the electrolyte containing the additive |
| CN109088099B (en) * | 2018-06-28 | 2021-01-26 | 华南师范大学 | Sulfonyl electrolyte additive giving consideration to high and low temperature performance and electrolyte containing additive |
| CN111276675A (en) * | 2018-12-04 | 2020-06-12 | 中国科学院宁波材料技术与工程研究所 | Modified silicon-carbon material and preparation method and application thereof |
| CN111276675B (en) * | 2018-12-04 | 2021-10-08 | 中国科学院宁波材料技术与工程研究所 | Modified silicon-carbon material and preparation method and application thereof |
| CN109802179A (en) * | 2019-01-03 | 2019-05-24 | 东莞市杉杉电池材料有限公司 | A kind of high-energy density ferrous phosphate lithium battery electrolyte and lithium ion battery |
| CN112467222A (en) * | 2020-10-23 | 2021-03-09 | 福建南平延平区南孚新能源科技有限公司 | Button secondary battery |
| CN112467222B (en) * | 2020-10-23 | 2022-09-16 | 福建南平延平区南孚新能源科技有限公司 | Button secondary battery |
| CN113823841A (en) * | 2021-10-29 | 2021-12-21 | 湖南法恩莱特新能源科技有限公司 | Electrolyte and preparation method and application thereof |
| CN113823841B (en) * | 2021-10-29 | 2023-11-28 | 湖南法恩莱特新能源科技有限公司 | Electrolyte and preparation method and application thereof |
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