CN103545551B - A kind of electrolyte being applicable to lithium titanate battery - Google Patents

A kind of electrolyte being applicable to lithium titanate battery Download PDF

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Publication number
CN103545551B
CN103545551B CN201310541045.5A CN201310541045A CN103545551B CN 103545551 B CN103545551 B CN 103545551B CN 201310541045 A CN201310541045 A CN 201310541045A CN 103545551 B CN103545551 B CN 103545551B
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electrolyte
carbonate
lithium salts
electrolyte according
phenylacetylene derivatives
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CN103545551A (en
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陈黎
甘朝伦
袁翔云
赵世勇
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Zhangjiagang Guotai Huarong New Chemical Materials Co Ltd
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Zhangjiagang Guotai Huarong New Chemical Materials Co Ltd
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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
    • 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 present invention relates to a kind of electrolyte being applicable to lithium titanate battery, comprise organic solvent and lithium salts, electrolyte also comprise in phenylacetylene derivatives one or more, phenylacetylene derivatives accounts for 0.05% ~ 10% of electrolyte quality, and the structural formula of phenylacetylene derivatives is: wherein, R 1, R 2, R 3independently selected from any one in hydrogen, hydroxyl, halogen, alkyl, alkoxyl, haloalkyl, halogenated alkoxy, alkylene, haloalkene alkyl, phenyl, halogenophenyl, xenyl, halogenated biphenyl base, phenylate base, triphenyl, halogeno-benzene ether, halo triphenyl, amido, ester group, cyano group, halogen is any one in F, Cl, Br, and halo is that part replaces or entirely replaces.The present invention, by adding phenylacetylene derivatives in the electrolytic solution, improves discharge capacity and the cycle life of lithium titanate battery, also suitably solves the bulging problem that lithium titanate battery occurs in cyclic process on the other hand.

Description

A kind of electrolyte being applicable to lithium titanate battery
Technical field
The present invention relates to a kind of lithium-ion battery electrolytes, particularly relate to the electrolyte in a kind of lithium ion battery taking lithium titanate as negative pole.
Background technology
Along with the fast development of portable electric appts, hybrid electric vehicle, electric automobile and space technology etc., secondary cell is had higher requirement in specific capacity, cycle life, fail safe etc.The lithium ion battery negative material of current actual extensive use is carbon-based material, because carbon negative pole material has the current potential very close with lithium metal, the easy precipitating metal Li dendrite of carbon electrodes and cause short circuit, thermal runaway etc. when the battery is overcharged, cause very large potential safety hazard thus to battery, particularly electrokinetic cell; During discharge and recharge simultaneously, lithium ion is embedding repeatedly and material with carbon element structure can made to be damaged in deintercalation process thus cause the decay of capacity.And with lithium titanate (Li 4ti 5o 12) material is that the lithium ion battery of negative pole overcomes the above problems well, Li 4ti 5o 12be 1.55V relative to the current potential of lithium electrode, not easily precipitating metal lithium, the fail safe of battery improves; Embed at Li or deviate from process, crystal formation does not change, and change in volume is less than 1%, is therefore called as " zero strain material ".Li 4ti 5o 12electrochemical diffusion coefficient be 2 × 10 -8cm 2/ s, an order of magnitude larger than the diffusion coefficient in carbon negative pole material, high diffusion coefficient make this negative material can fast, multi cycle discharge and recharge.But current lithium titanate anode material reacts with electrolyte in charge and discharge process, decompose and produce gas, discharge nowhere and cause inflatable, and then the capacity affecting battery plays and circulating effect.
Summary of the invention
Technical problem to be solved by this invention is to provide and a kind ofly improves the discharge capacity of lithium titanate battery and the electrolyte being applicable to lithium titanate battery of cycle life.
For achieving the above object, the technical solution used in the present invention is:
A kind of electrolyte being applicable to lithium titanate battery, comprise organic solvent and lithium salts, described electrolyte also comprise in phenylacetylene derivatives one or more, described phenylacetylene derivatives accounts for 0.05% ~ 10% of described electrolyte quality, and the structural formula of described phenylacetylene derivatives is:
Wherein, R 1, R 2, R 3independently selected from any one in hydrogen, hydroxyl, halogen, alkyl, alkoxyl, haloalkyl, halogenated alkoxy, alkylene, haloalkene alkyl, phenyl, halogenophenyl, xenyl, halogenated biphenyl base, phenylate base, triphenyl, halogeno-benzene ether, halo triphenyl, amido, ester group, cyano group, described halogen is any one in F, Cl, Br, and described halo is that part replaces or entirely replaces.
Preferably, described phenylacetylene derivatives accounts for 0.5% ~ 1% of described electrolyte quality.
Preferably, described phenylacetylene derivatives is in any one or multiple.
Particularly, described organic solvent is one or more in carbonic ester, carboxylate, ether, sulfone.
More specifically, described carbonic ester is one or more in ethylene carbonate, propene carbonate, butylene carbonate base ester, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, propene carbonate; Described carboxylate is one or more in methyl formate, Ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate, ethyl butyrate; Described ether is one or more in dimethoxymethane, 1,2-dimethoxy-ethane, oxolane, DOX; Described sulfone is one or more in methyl-sulfoxide, sulfolane, dimethyl sulfone.
Particularly, described lithium salts is LiPF 6, LiBF 4, LiClO 4, CF 3sO 3li, LiCH 3sO 3, LiSCN, LiNO 3, LiO 3sCF 2cF 3, LiAsF 6, LiAlCl 4, one or more in LiTFSI, LiFSI.
Preferably, the concentration of described lithium salts is 0.7 ~ 1.5mol/L.
More preferably, the concentration of described lithium salts is 0.9 ~ 1.2mol/L.
Preferably, described electrolyte also comprises film for additive, and described film for additive accounts for 0.05% ~ 5% of described electrolyte quality.
More preferably, described film for additive accounts for 0.8% ~ 2.0% of described electrolyte quality.
Particularly, described film for additive is vinylene carbonate, vinylethylene carbonate, ethylene sulfite, propylene sulfite, vinyl ethylene sulfite, fluorinated ethylene carbonate, 1, one or more in 3-sulfonic acid propiolactone, Isosorbide-5-Nitrae-sulfonic acid butyrolactone, LiBOB, LiODFB.
Because technique scheme is used, the present invention compared with prior art has following advantages:
The present invention, by adding phenylacetylene derivatives in the electrolytic solution, improves discharge capacity and the cycle life of lithium titanate battery, also suitably solves the bulging problem that lithium titanate battery occurs in cyclic process on the other hand.
Embodiment
Below in conjunction with specific embodiment, the present invention is elaborated:
Comparative example 1
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, obtains electrolyte.
Comparative example 2
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite of 1%, obtain electrolyte.
Comparative example 3
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite of 1% and the LiBOB of 1% respectively, obtain electrolyte.
Embodiment 1
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the 3-difluoro-methoxy phenylacetylene of 1% obtain electrolyte.
Embodiment 2
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the 3-cyano group-4-Methoxy-phenylacetylene of 1% obtain electrolyte.
Embodiment 3
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the 2-acetylene aniline of 1% obtain electrolyte.
Embodiment 4
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the 3-hydroxy phenyl acetylene of 1% obtain electrolyte.
Embodiment 5
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite and 1% of 1% obtain electrolyte.
Embodiment 6
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/diethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite and 1% of 1% obtain electrolyte.
Embodiment 7
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/diethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite and 1% of 1% obtain electrolyte.
Embodiment 8
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/diethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite and 1% of 1% obtain electrolyte.
Embodiment 9
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite of 1%, the LiBOB and 1% of 1% respectively obtain electrolyte.
Embodiment 10
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite of 1%, the LiBOB and 1% of 1% respectively obtain electrolyte.
Embodiment 11
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite of 1%, the LiBOB and 1% of 1% respectively obtain electrolyte.
Embodiment 11
By lithium salts (LiPF 6) be dissolved in the mixed solvent of ethylene carbonate/methyl ethyl carbonate/dimethyl carbonate/propene carbonate (mass ratio is 30/55/10/5) and obtain mixed solution, wherein LiPF 6concentration is 1mol/L, in this mixed solution, calculates by electrolyte gross mass, adds the vinyl ethylene sulfite of 1%, the LiBOB and 1% of 1% respectively obtain electrolyte.
Experimental result
Normal-temperature circulating performance is tested:
Adopt the cycle performance of Shenzhen new prestige cell tester test battery.
Electrolyte after the configuration of comparative example 1, comparative example 2, comparative example 3 and embodiment 1 to 11 is injected the lithium titanate duricrust battery with batch same model, test battery is under 0 ~ 3V, normal temperature environment carries out the cycle performance test of 1C, and before and after normal temperature circulation volume conservation rate and circulation, thickness comparing data is as shown in table 1.
Table 1
As shown in Table 1, the lithium titanate battery that the lithium titanate battery that prepared by electrolyte of the present invention is prepared at the electrolyte that cycle life and the cell thickness expansion rate of 0 ~ 3V, 1C rate charge-discharge are obviously better than comparative example; Further, embodiment 9 wherein has extremely significantly advantage especially in circulating battery conservation rate and cell expansion degree.
Above-described embodiment is only for illustrating technical conceive of the present invention and feature; its object is to person skilled in the art can be understood content of the present invention and implement according to this; can not limit the scope of the invention with this; all equivalences done according to Spirit Essence of the present invention change or modify, and all should be encompassed within protection scope of the present invention.

Claims (9)

1. one kind is applicable to the electrolyte of lithium titanate battery, comprise organic solvent and lithium salts, it is characterized in that: described electrolyte also comprise in phenylacetylene derivatives one or more, described phenylacetylene derivatives accounts for 0.05% ~ 10% of described electrolyte quality, and described phenylacetylene derivatives is , , , in any one or multiple.
2. electrolyte according to claim 1, is characterized in that: described phenylacetylene derivatives accounts for 0.5% ~ 1% of described electrolyte quality.
3. electrolyte according to claim 1, is characterized in that: described organic solvent is one or more in carbonic ester, carboxylate, ether, sulfone.
4. electrolyte according to claim 3, is characterized in that: described carbonic ester is one or more in ethylene carbonate, propene carbonate, butylene carbonate base ester, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate; Described carboxylate is one or more in methyl formate, Ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate, ethyl butyrate; Described ether is one or more in dimethoxymethane, 1,2-dimethoxy-ethane, oxolane, DOX; Described sulfone is one or more in methyl-sulfoxide, sulfolane, dimethyl sulfone.
5. electrolyte according to claim 1, is characterized in that: described lithium salts is LiPF 6, LiBF 4, LiClO 4, CF 3sO 3li, LiCH 3sO 3, LiSCN, LiNO 3, LiO 3sCF 2cF 3, LiAsF 6, LiAlCl 4, one or more in LiTFSI, LiFSI.
6. electrolyte according to claim 1, is characterized in that: the concentration of described lithium salts is 0.7 ~ 1.5mol/L.
7. electrolyte according to claim 6, is characterized in that: the concentration of described lithium salts is 0.9 ~ 1.2mol/L.
8. electrolyte according to claim 1, is characterized in that: described electrolyte also comprises film for additive, and described film for additive accounts for 0.05% ~ 5% of described electrolyte quality.
9. electrolyte according to claim 8, it is characterized in that: described film for additive is vinylene carbonate, vinylethylene carbonate, ethylene sulfite, propylene sulfite, vinyl ethylene sulfite, fluorinated ethylene carbonate, 1, one or more in 3-sulfonic acid propiolactone, Isosorbide-5-Nitrae-sulfonic acid butyrolactone, LiBOB, LiODFB.
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CN105098238A (en) * 2014-05-20 2015-11-25 宁德时代新能源科技有限公司 Lithium ion secondary battery and electrolyte thereof
CN104900917A (en) * 2015-07-09 2015-09-09 上海动力储能电池***工程技术有限公司 Electrolyte for lithium titanate lithium ion battery
CN105098241A (en) * 2015-07-13 2015-11-25 新余学院 Electrolyte solution compatible with lithium-ion battery anode material lithium titanate
CN107394270A (en) * 2017-07-26 2017-11-24 天津银隆新能源有限公司 Electrolyte for improving lithium titanate battery cyclical stability and preparation method thereof
CN109994775B (en) * 2017-12-29 2022-01-18 张家港市国泰华荣化工新材料有限公司 Lithium battery
CN113748553B (en) * 2019-05-30 2024-02-09 松下知识产权经营株式会社 Nonaqueous electrolyte secondary battery
CN111640989A (en) * 2020-07-24 2020-09-08 天津市捷威动力工业有限公司 Electrolyte for reducing gas generation of lithium titanate battery cell

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