CN103633372A - Fire-resistant lithium-ion battery electrolyte - Google Patents

Fire-resistant lithium-ion battery electrolyte Download PDF

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CN103633372A
CN103633372A CN201310588998.7A CN201310588998A CN103633372A CN 103633372 A CN103633372 A CN 103633372A CN 201310588998 A CN201310588998 A CN 201310588998A CN 103633372 A CN103633372 A CN 103633372A
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salt
tfsi
methyl
bis trifluoromethyl
electrolyte
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CN103633372B (en
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高昆
李姝�
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Shaanxi Normal University
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Shaanxi Normal University
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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
    • 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
    • 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
    • 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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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

The invention provides a safe lithium-ion battery electrolyte which comprises an electrolyte salt, an organic solvent and a catenarian quaternary ammonium salt ionic liquid. According to the invention, through selecting a specific type of organic solvent and ionic liquid which are mixed in different proportions, the volatility of the electrolyte can be reduced, and a battery filled with the electrolyte does not generate smoke and fire when being overcharged, so that the fire resistance and use security of the electrolyte can be improved effectively.

Description

A kind of anti-combustion type lithium-ion battery electrolytes
Technical field
The present invention relates to lithium-ion battery electrolytes field, relate to a kind of use of novel ion liquid.
Background technology
Lithium-ion battery electrolytes is the important component part of battery, is bearing the effect of transmitting electric charge between both positive and negative polarity in battery.It plays vital effect to the specific capacity of battery, operating temperature range, cycle efficieny and security performance etc.Volatile, the inflammable carbonates organic solvent that mostly is owing to using in traditional organic electrolyte, has affected the fail safe of battery.Ionic liquid refers to all and is comprised of ion, at room temperature presents liquid material, claims again ionic liquid at room temperature or room temperature fused salt.It has following physicochemical properties: steam forces down, not volatile, nonflammable, high thermal stability, high conductivity, electrochemical window are wide, may for solving that the safety issue of lithium ion battery provides.
At present, the application of traditional organic electrolyte is very wide, but the destabilizing factors such as electrolyte is inflammable, easy decomposition have limited further developing of it.Scientists has been carried out a large amount of improvement research for this defect.Wherein, the related work that relates to ionic liquid application mainly contains: gondola C.Arbizzani etc. have studied ionic liquid N-methyl-N-butyl pyrroles bis trifluoromethyl sulfimide salt (PY 14-TFSI) application in lithium ion battery.By research, find, work as PY 14-TFSI and organic solvent mass ratio are 1:1 while mixing, and the burning degree of the electrolyte of this mixing has dropped to minimum.Germany A.Balducci etc. has studied 0.3M LiTFSI and N-methyl-N-butyl pyrroles bis trifluoromethyl sulfimide salt (PYR 14physical and chemical performance and chemical property while TFSI) doing mixed electrolytic solution with propene carbonate (PC), and find by its thermogravimetric (TG) curve: PYR 14adding of TFSI makes the decomposition temperature of PC be elevated to 400 ℃ nearly from 150 ℃ of left and right.And when ionic liquid content is 80%, mixed electrolyte has showed obvious noninflammability.Similar in this, the contrast such as the J.Mun of Korea S graphite cathode material is respectively at N-methyl-N-propyl pyrrole bis trifluoromethyl sulfimide salt (PYR 13tFSI) the thermogravimetric analysis curve in ionic liquid and ethylene carbonate and diethyl carbonate organic solvent.Result shows: in organic solvent, the temperature that exothermic peak occurs is between 150～230 ℃, and the exothermic peak of ionic liquid just occurs when being greater than 250 ℃, and the total amount of heat in the middle of the total amount of heat of emitting between 150～350 ℃ is significantly less than organic solvent.In addition, Canadian A.Guerfi and Polish A.Lewandowski have done comparative study to imidazoles and piperidines ionic liquid and organic solvent mixed electrolytic solution respectively, find when mass ratio that ionic liquid accounts for whole electrolyte is greater than 40%, electrolyte can not burn, the safety index that meets electrolyte, can improve the security performance of electrolyte.This type of research of China, progress a little later.The Yin Ge equality of Harbin Institute of Technology has been added 1-methyl isophthalic acid-propyl group piperidines bis trifluoromethyl sulfimide salt (PP of 50% in organic electrolyte 13tFSI), after and 2% di-oxalate lithium borate (LiBOB), glass fibre bar burns hardly.Presentation of results, PP 13the use of TFSI and LiBOB can improve the fail safe of mixed electrolytic solution.The Xiang Hongfa of Chinese University of Science and Technology etc. joins traditional LiPF using dimethyl methyl phosphonate (DMMP) as flame-retardant additive 6in organic electrolyte, result of study shows, with 1M LiPF 6/ EC+DEC electrolyte is compared, and having added the later electrolyte of DMMP has had large increase in the redox reaction stability of electrode surface, thereby has improved the fail safe of lithium ion battery.These research work absolutely prove: the use of ionic liquid can improve the serviceability temperature scope of lithium-ion battery electrolytes, and can effectively improve the security performance of electrolyte.
Ionic liquid of the present invention is 1-dimethyl-1-ethyl-1-butyl quaternary ammonium salt bis trifluoromethyl sulfimide salt (N 1124-TFSI).Except having the advantage that low viscosity, high electricity lead, N 1124the most significant feature of-TFSI is that electrochemical window is wide, and Heat stability is good is beneficial to and improves its use and performance in battery.
Summary of the invention
The present invention provides a kind of anti-combustion type lithium-ion battery electrolytes for improving the fail safe of ion battery, comprise electrolytic salt, organic solvent and ion liquid of quaternaries, described organic solvent comprises dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (EMC), ethylene carbonate (EC), propene carbonate (PC).
Further, the weight content of ionic liquid is organic solvent 20%～80%.
Further, organic solvent is comprised of ethylene carbonate and diethyl carbonate.
Further, described ionic liquid comprises one or more in following material: 1-methyl-3-hexyl imidazoles methyl fluoride sulfimide salt (EMI-FSI), 1-methyl-3-hexyl imidazoles bis trifluoromethyl sulfimide salt (EMI-TFSI), 1-methyl isophthalic acid-propyl pyrrole alkane methyl fluoride sulfimide salt (PY 13-FSI), 1-butyl-2,3-methylimidazole bis trifluoromethyl sulfimide salt (BMMI-TFSI), 1-methyl isophthalic acid-propyl group piperidines bis trifluoromethyl sulfimide salt (PP 13-TFSI), 1-methyl isophthalic acid-propyl group piperidines methyl fluoride sulfimide salt (PP 13-FSI), 1-methyl isophthalic acid-butyl piperidine bis trifluoromethyl sulfimide salt (PP 14-TFSI), 1-methyl isophthalic acid-butyl piperidine methyl fluoride sulfimide salt (PP 14-FSI), 1-trimethyl-1-butyl quaternary ammonium salt bis trifluoromethyl sulfimide salt (N 1144-TFSI), 1-dimethyl-1-ethyl-1-butyl quaternary ammonium salt bis trifluoromethyl sulfimide salt (N 1124-TFSI), 1-trimethyl-1-hexyl quaternary ammonium salt bis trifluoromethyl sulfimide salt (N 1116-TFSI).
Further, described ion liquid of quaternaries is 1-dimethyl-1-ethyl-1-butyl quaternary ammonium salt bis trifluoromethyl sulfimide salt.
Further, described electrolytic salt is LiPF 6, concentration is 0.4～1.0mol/kg.
The present invention also provides a kind of lithium ion battery, contains above-mentioned electrolyte.
Accompanying drawing explanation
By describing in more detail exemplary embodiment of the present invention with reference to accompanying drawing, above and other aspect of the present invention and advantage will become and more be readily clear of, in the accompanying drawings:
Fig. 1 is manganate cathode material for lithium 50 cyclic discharge capacity figure in D bottle electrolyte in embodiment 1;
Fig. 2 is the differential scanning calorimetric curve of D bottle electrolyte in business electrolyte and embodiment 1.
Embodiment
Hereinafter, now with reference to accompanying drawing, the present invention is described more fully, various embodiment shown in the drawings.Yet the present invention can implement in many different forms, and should not be interpreted as being confined to embodiment set forth herein.On the contrary, it will be thorough with completely providing these embodiment to make the disclosure, and scope of the present invention is conveyed to those skilled in the art fully.
Fig. 1 is manganate cathode material for lithium 50 cyclic discharge capacity figure in D bottle electrolyte in embodiment 1; With business electrolysis liquid phase ratio, use D bottle electrolyte (LiPF 6/ N 1124first section of discharge capacity of LiMn2O4 test battery TFSI+EC-DEC) is lower slightly, this and N 1124tFSI adds the viscosity of rear electrolyte to increase, thereby has reduced relevant with the wetting property of solid state electrode.Then, the two capacity moves closer to.Fig. 2 is the differential scanning calorimetric curve of D bottle electrolyte in business electrolyte and embodiment 1.In the curve comparison showing at Fig. 2, can see: in business electrolyte system, the decomposing thermal spike of EC-DEC organic solvent appears at 230 ℃-300 ℃.And in embodiment 1 in D bottle electrolyte system, due to ionic liquid N 1124the increase of TFSI composition, the decomposition temperature of EC-DEC is delayed 314 ℃, and a minute heat of desorption for ionic liquid composition appears at 368 ℃ of left and right.The anti-combustion of whole electrolyte and thermal stability have obtained significantly improving.
Embodiment 1: in glove box, prepare electrolyte, totally 500 grams of EC:DEC=3:7 (wt%), respectively get 100 grams and be sub-packed in polytetrafluoroethylene bottle, are designated as respectively A, B, C, D, E.Wherein
A bottle: add 40% (wt%) N 1124-TFSI and 16.73 grams of LiPF 6, making lithium salt is 0.6mol/kg.
B bottle: add 50% (wt%) N 1124-TFSI and 20.07 grams of LiPF 6, making lithium salt is 0.6mol/kg.
C bottle: add 60% (wt%) N 1124-TFSI and 25.09 grams of LiPF 6, making lithium salt is 0.6mol/kg.
D bottle: add 70% (wt%) N 1124-TFSI and 33.45 grams of LiPF 6, making lithium salt is 0.6mol/kg.
E bottle: add 80% (wt%) N 1124-TFSI and 50.18 grams of LiPF 6, making lithium salt is 0.6mol/kg.
Embodiment 2: in glove box, prepare electrolyte, totally 500 grams of EC:DEC=4:6 (wt%), respectively get 100 grams and be sub-packed in polytetrafluoroethylene bottle, are designated as respectively A, B, C, D, E.Wherein
A bottle: add 40% (wt%) N 1124-TFSI and 16.73 grams of LiPF 6, making lithium salt is 0.6mol/kg.
B bottle: add 50% (wt%) N 1124-TFSI and 20.07 grams of LiPF 6, making lithium salt is 0.6mol/kg.
C bottle: add 60% (wt%) N 1124-TFSI and 25.09 grams of LiPF 6, making lithium salt is 0.6mol/kg.
D bottle: add 70% (wt%) N 1124-TFSI and 33.45 grams of LiPF 6, making lithium salt is 0.6mol/kg.
E bottle: add 80% (wt%) N 1124-TFSI and 50.18 grams of LiPF 6, making lithium salt is 0.6mol/kg.
Embodiment 3: in glove box, prepare electrolyte, totally 500 grams of EC:DEC=5:5 (wt%), respectively get 100 grams and be sub-packed in polytetrafluoroethylene bottle, are designated as respectively A, B, C, D, E.Wherein
A bottle: add 40% (wt%) N 1124-TFSI and 16.73 grams of LiPF 6, making lithium salt is 0.6mol/kg.
B bottle: add 50% (wt%) N 1124-TFSI and 20.07 grams of LiPF 6, making lithium salt is 0.6mol/kg.
C bottle: add 60% (wt%) N 1124-TFSI and 25.09 grams of LiPF 6, making lithium salt is 0.6mol/kg.
D bottle: add 70% (wt%) N 1124-TFSI and 33.45 grams of LiPF 6, making lithium salt is 0.6mol/kg.
E bottle: add 80% (wt%) N 1124-TFSI and 50.18 grams of LiPF 6, making lithium salt is 0.6mol/kg.
Embodiment 4: in glove box, prepare electrolyte, totally 500 grams of EC:DEC=6:4 (wt%), respectively get 100 grams and be sub-packed in polytetrafluoroethylene bottle, are designated as respectively A, B, C, D, E.Wherein
A bottle: add 40% (wt%) N 1124-TFSI and 16.73 grams of LiPF 6, making lithium salt is 0.6mol/kg.
B bottle: add 50% (wt%) N 1124-TFSI and 20.07 grams of LiPF 6, making lithium salt is 0.6mol/kg.
C bottle: add 60% (wt%) N 1124-TFSI and 25.09 grams of LiPF 6, making lithium salt is 0.6mol/kg.
D bottle: add 70% (wt%) N 1124-TFSI and 33.45 grams of LiPF 6, making lithium salt is 0.6mol/kg.
E bottle: add 80% (wt%) N 1124-TFSI and 50.18 grams of LiPF 6, making lithium salt is 0.6mol/kg.
Embodiment 5: in glove box, prepare electrolyte, totally 500 grams of EC:DEC=7:3 (wt%), respectively get 100 grams and be sub-packed in polytetrafluoroethylene bottle, are designated as respectively A, B, C, D, E.Wherein
A bottle: add 40% (wt%) N 1124-TFSI and 16.73 grams of LiPF 6, making lithium salt is 0.6mol/kg.
B bottle: add 50% (wt%) N 1124-TFSI and 20.07 grams of LiPF 6, making lithium salt is 0.6mol/kg.
C bottle: add 60% (wt%) N 1124-TFSI and 25.09 grams of LiPF 6, making lithium salt is 0.6mol/kg.
D bottle: add 70% (wt%) N 1124-TFSI and 33.45 grams of LiPF 6, making lithium salt is 0.6mol/kg.
E bottle: add 80% (wt%) N 1124-TFSI and 50.18 grams of LiPF 6, making lithium salt is 0.6mol/kg.
The foregoing is only embodiments of the invention, be not limited to the present invention.The present invention can have various suitable changes and variation.All any modifications of doing within the spirit and principles in the present invention, be equal to replacement, improvement etc., within protection scope of the present invention all should be included in.

Claims (7)

1. an anti-combustion type lithium-ion battery electrolytes, comprises electrolytic salt, organic solvent and ion liquid of quaternaries, it is characterized in that:
Described organic solvent comprises dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (EMC), ethylene carbonate (EC), propene carbonate (PC).
2. according to ionic liquid described in claim 1, it is characterized in that: the weight content of ionic liquid is organic solvent 20%～80%.
3. according to organic solvent described in claim 1 or 2, it is characterized in that: organic solvent is comprised of ethylene carbonate and diethyl carbonate.
4. according to the lithium-ion battery electrolytes described in claim 1, it is characterized in that: described ionic liquid comprises one or more in following material: 1-methyl-3-hexyl imidazoles methyl fluoride sulfimide salt (EMI-FSI), 1-methyl-3-hexyl imidazoles bis trifluoromethyl sulfimide salt (EMI-TFSI), 1-methyl isophthalic acid-propyl pyrrole alkane methyl fluoride sulfimide salt (PY 13-FSI), 1-butyl-2,3-methylimidazole bis trifluoromethyl sulfimide salt (BMMI-TFSI), 1-methyl isophthalic acid-propyl group piperidines bis trifluoromethyl sulfimide salt (PP 13-TFSI), 1-methyl isophthalic acid-propyl group piperidines methyl fluoride sulfimide salt (PP 13-FSI), 1-methyl isophthalic acid-butyl piperidine bis trifluoromethyl sulfimide salt (PP 14-TFSI), 1-methyl isophthalic acid-butyl piperidine methyl fluoride sulfimide salt (PP 14-FSI), 1-trimethyl-1-butyl quaternary ammonium salt bis trifluoromethyl sulfimide salt (N 1114-TFSI), 1-dimethyl-1-ethyl-1-butyl quaternary ammonium salt bis trifluoromethyl sulfimide salt (N 1124-TFSI), 1-trimethyl-1-hexyl quaternary ammonium salt bis trifluoromethyl sulfimide salt (N 1116-TFSI).
5. according to the ionic liquid described in claim 2, it is characterized in that: described ion liquid of quaternaries is 1-dimethyl-1-ethyl-1-butyl quaternary ammonium salt bis trifluoromethyl sulfimide salt.
6. according to the lithium-ion battery electrolytes described in claim 1, it is characterized in that: described electrolytic salt is LiPF 6, concentration is 0.4～1.0mol/kg.
7. a lithium ion battery, is characterized in that: contain the electrolyte described in above-mentioned any one claim.
CN201310588998.7A 2013-11-20 2013-11-20 A kind of anti-combustion type lithium-ion battery electrolytes Expired - Fee Related CN103633372B (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110364764A (en) * 2019-07-23 2019-10-22 浙江大学 A kind of electrolyte and preparation method thereof for lithium ion battery

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