CN104112869A - Nonaqueous electrolyte additive capable of improving high-temperature impedance performance of manganese-contained lithium ion battery - Google Patents

Nonaqueous electrolyte additive capable of improving high-temperature impedance performance of manganese-contained lithium ion battery Download PDF

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Publication number
CN104112869A
CN104112869A CN201310135140.5A CN201310135140A CN104112869A CN 104112869 A CN104112869 A CN 104112869A CN 201310135140 A CN201310135140 A CN 201310135140A CN 104112869 A CN104112869 A CN 104112869A
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China
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electrolyte
ion battery
lithium ion
lithium
manganese
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CN201310135140.5A
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冯力
张勤
徐建平
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Jiangsu Highstar Battery Manufacturing Co., Ltd.
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NANTONG LIHE NEW ENERGY 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

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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)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Physics & Mathematics (AREA)
  • Materials Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)

Abstract

The invention provides a nonaqueous electrolyte additive capable of improving a high-temperature impedance performance of a manganese-contained lithium ion battery. An electrolyte consists of four types of components: a lithium salt, a nonaqueous organic solvent, a stabilizing additive and other functional additives. The lithium salt is one or more of compounds having following molecular formulas such as LiPF6, LiBF4, LiBOB, LiClO4 and LiPF3(C2F5)3. The stabilizing additive is selected from more than one in the group consisting of tris(trimethylsilyl)phosphate, monoethanolamine and methylene methanedisulfonate. An addition amount of the stabilizing additive accounts for 0.1-5% of a total weight of the electrolyte. The electrolyte is used for manufacturing a lithium ion battery in which a cathode active material employs spinel lithium manganates or a mixture composed of the spinel lithium manganates and lithium nickel cobaltate manganese oxide. Through addition of an ester containing phosphorus or sulphur and an alcohol amine-typed stabilizing agent, storage performances, such as a high-temperature impedance performance and the like, of the manganese-contained lithium ion battery are improved.

Description

A kind of non-water electrolytic solution additive improving containing manganese high-temperature lithium ion battery impedance behavior
[technical field]
The present invention relates to the additive that a kind of nonaqueous electrolytic solution the coupling that can further improve containing the high temperature impedance behavior of manganese lithium ion battery has special stabilization function, belong to material technology field.
[background technology]
Along with the development of Study on Li-ion batteries using and development technique, people wish to improve the performance that is widely used of battery when reducing costs.Nickle cobalt lithium manganate ternary material mixes the important research direction that becomes current raising performance of lithium ion battery and reduce costs as anode active material of lithium ion battery with spinel lithium manganate.Nickel-cobalt lithium manganate cathode material combines LiCoO 2, LiNiO 2and LiMnO 2the advantages such as specific energy and specific power performance, Stability Analysis of Structures.Spinel lithium manganate has three-dimensional tunnel structure, and the de-embedding of lithium ion is convenient, and manganese aboundresources, cheap, environmentally friendly, safe, is suitable as anode material for lithium-ion batteries.But spinel lithium manganate battery in use, especially under hot conditions, capacity attenuation and impedance increase are particularly serious, and its main cause is the dissolving of manganese ion in spinel structure, and move on graphite cathode surface and deposit, make negative pole poisoning, surface electrochemistry reduced activity.Electrolyte is the direct explosive train that causes ageing of performance to the corrosion of lithium manganate material.On the other hand, use the battery of common electrolyte at high temperature, electrode surface SEI (solid electrolyte interface) perforated membrane poor stability, easily causes electrode resistance to increase, battery charging and discharging hydraulic performance decline and the lost of life.Therefore, need to select to add the additive with special stabilization function to suppress degenerating of this material surface characteristic, particularly under high ambient conditions.
Lithium-ion battery electrolytes is comprised of lithium salts and non-aqueous organic solvent conventionally, and commercial electrolyte adds some known functional additives conventionally, has good SEI filming performance after battery is changed into, but chemistry and physical mechanical stability also need further raising.U.S. Patent No. 5,626, points out to add additive agent electrolyte vinylene carbonate can form stable solid electrolyte perforated membrane in 981, thereby improves battery performance.In Japan Patent No.11-269196, think and add the electrolyte containing three (trimethyl silane) phosphate ester additive, can improve LiCoO 2the high temperature cyclic performance of anodal lithium ion battery.Therefore develop electrolyte for lithium ion battery, and coupling having additive, the especially stability under high ambient conditions of special stabilization function, is all that tool is of great significance for improving high-temperature lithium ion battery storage life.
[summary of the invention]
Technical problem to be solved by this invention is, provide a kind of and can further improve the additive that the electrolyte that increases containing the high temperature impedance of manganese lithium ion battery coupling have special stabilization function, in this electrolyte, due to the adding of stabilization additives, improved battery electrode surface SEI (solid electrolyte interface) perforated membrane stability.In addition, may effectively control reaction rate and the manganese concentration of metal ions on electrode surface such as organic solvent composition in electrolyte and water, acid, use the high temperature impedance containing manganese lithium ion battery prepared by this electrolyte increase be improved significantly.
The present invention is achieved through the following technical solutions:
Under high temperature resistance, the aging manganese lithium-ion battery electrolytes that contains also mates a stabilization additives with specific function, and this electrolyte is comprised of four constituents: lithium salts, non-aqueous organic solvent, stabilization additives and other functional additives.
Described lithium salts molecular formula is one or more mixtures in following compound: LiPF 6, LiBOB, LiBF 4, LiPF 3(C 2f 5) 3, LiClO 4.
Described can be 18650 column types or folded formula profile containing manganese lithium ion battery.
Described stabilization additives is selected from more than one combinations in three (trimethyl silane) phosphate, methane-disulfonic acid methylene ester, monoethanolamine, and the addition of stabilization additives is 0.1%～5% of electrolyte total weight.The purposes of described electrolyte is applied to manufacture take and contains the lithium ion battery that manganese active material is positive electrode, containing manganese active material, be wherein the mixture of nickel, cobalt, manganese ternary oxidate for lithium material and spinel lithium manganate, spinel lithium manganate weight accounts for 10%～100% of positive electrode active materials total weight.
The invention has the beneficial effects as follows: containing in manganese lithium-ion battery electrolytes, adding stabilization additives, can improve lithium ion battery negative surface SEI (solid electrolyte interface) perforated membrane stability.Also can control the acidity value in electrolyte, effectively reduce the erosion of electrolyte to positive electrode, prevent that it from depositing in negative terminal surface, and reduce negative reaction generation etc., thereby suppress the electrode performance acceleration decay that impedance is risen and caused, improve the high-temperature storage performance containing manganese lithium ion battery.
[embodiment]
Below in conjunction with embodiment and subordinate list, the present invention is described in further detail; these specific embodiments are the preferred embodiments of the present invention; can not limit claim of the present invention; the present invention still has multiple other concrete execution mode; all employings are equal to replacement or equivalent transformation and all technical schemes of forming, within all belonging to the scope of protection of present invention.
Comparative example 1:
By lithium salts LiPF 6be dissolved in the mixed solvent of ethylene carbonate, propene carbonate, dimethyl carbonate, methyl ethyl carbonate, wherein ethylene carbonate: propene carbonate: dimethyl carbonate: the mass ratio of methyl ethyl carbonate is 3: 1: 3: 3, LiPF 6concentration be 1mol/L.Then in this solution, by 2% of electrolyte total weight, add vinylene carbonate, make contrast electrolyte.This electrolyte is applied in lithium ion battery that LiMn2O4 weight accounts for positive electrode active materials total weight 100%.
Embodiment 1:
By lithium salts LiPF 6be dissolved in the mixed solvent of ethylene carbonate, propene carbonate, methyl ethyl carbonate, diethyl carbonate, wherein ethylene carbonate: propene carbonate: methyl ethyl carbonate: the mass ratio of diethyl carbonate is 3: 1: 3: 3, LiPF 6concentration be 1mol/L.Then in this solution, by 2% of electrolyte total weight, add vinylene carbonate, by 1% of electrolyte total weight, add monoethanolamine, by 1% of electrolyte total weight, add three (trimethyl silane) phosphate, make required electrolyte.This electrolyte is applied in lithium ion battery that LiMn2O4 weight accounts for positive electrode active materials total weight 100%.
Embodiment 2:
By lithium salts LiPF 6be dissolved in the mixed solvent of ethylene carbonate, propene carbonate, methyl ethyl carbonate, diethyl carbonate, wherein ethylene carbonate: propene carbonate: methyl ethyl carbonate: the mass ratio of diethyl carbonate is 3: 1: 3: 3, LiPF 6concentration be 1.0mol/L.Then in this solution, by 2% of electrolyte total weight, add vinylene carbonate, by 1.5% of electrolyte total weight, add monoethanolamine, by 2.5% of electrolyte total weight, add three (trimethyl silane) phosphate, make required electrolyte.This electrolyte is applied in lithium ion battery that LiMn2O4 weight accounts for positive electrode total weight 100%.
Embodiment 3:
By lithium salts LiPF 6be dissolved in the mixed solvent of ethylene carbonate, propene carbonate, methyl ethyl carbonate, diethyl carbonate, wherein ethylene carbonate: propene carbonate: methyl ethyl carbonate: the mass ratio of diethyl carbonate is 3: 1: 3: 3, LiPF 6concentration be 1.0mol/L.Then in this solution, by 2% of electrolyte total weight, add vinylene carbonate, by 1% of electrolyte total weight, add monoethanolamine, by 1% of electrolyte total weight, add methane-disulfonic acid methylene ester, make required electrolyte.This electrolyte is applied in lithium ion battery that LiMn2O4 weight accounts for positive electrode total weight 100%.
Embodiment 4:
By lithium salts LiPF 6be dissolved in the mixed solvent of ethylene carbonate, propene carbonate, methyl ethyl carbonate, diethyl carbonate, wherein ethylene carbonate: propene carbonate: methyl ethyl carbonate: the mass ratio of diethyl carbonate is 3: 1: 3: 3, LiPF 6concentration be 1mol/L.Then in this solution, by 2% of electrolyte total weight, add vinylene carbonate, by 1.5% of electrolyte total weight, add monoethanolamine, by 2.5% of electrolyte total weight, add methane-disulfonic acid methylene ester, make required electrolyte.This electrolyte is applied in lithium ion battery that LiMn2O4 weight accounts for positive electrode total weight 100%.
Embodiment 5:
By lithium salts LiPF 6be dissolved in the mixed solvent of ethylene carbonate, propene carbonate, methyl ethyl carbonate, dimethyl carbonate, wherein ethylene carbonate: propene carbonate: methyl ethyl carbonate: the mass ratio of diethyl carbonate is 3: 1: 3: 3, LiPF 6concentration be 1mol/L.Then in this solution, by 2% of electrolyte total weight, add vinylene carbonate, by 1% of electrolyte total weight, add monoethanolamine, by 2% of electrolyte total weight, add methane-disulfonic acid methylene ester, make required electrolyte.This electrolyte is applied in lithium ion battery that LiMn2O4 weight accounts for positive electrode total weight 35%.
Result of implementation is as follows:
Table 1 is for selecting the electrolyte of comparative example 1, embodiment 1 and example 2 and containing Different Weight stabilization additives three (trimethyl silane) phosphate and monoethanolamine is made containing manganese lithium ion 18650 cylindrical batteries, at 60 ℃ ± 2 ℃, 60% charged storage is 30 days, then the institute's impedance of surveying increase (%) before and after storing is contrasted.In manganese lithium ion battery, spinel lithium manganate and nickle cobalt lithium manganate active anode compartment material weight percentage are 100/0
Table 2 is for selecting the electrolyte of comparative example 1, embodiment 1 and example 2 and containing Different Weight stabilization additives methane-disulfonic acid methylene ester and monoethanolamine is made containing manganese lithium ion 18650 cylindrical batteries, at 60 ℃ ± 2 ℃, 60% charged storage is 30 days, then the institute's impedance of surveying increase (%) before and after storing is contrasted.In manganese lithium ion battery, spinel lithium manganate and nickle cobalt lithium manganate active anode compartment material weight percentage are 100/0
Table 3 is for selecting the electrolyte of comparative example 1, embodiment 1 and containing Different Weight stabilization additives methane-disulfonic acid methylene ester and monoethanolamine is made containing manganese lithium ion 18650 cylindrical batteries, at 60 ℃ ± 2 ℃, 60% charged storage is 30 days, then the institute's impedance of surveying increase (%) before and after storing is contrasted.In manganese lithium ion battery, spinel lithium manganate and nickle cobalt lithium manganate active anode compartment material weight percentage are 35/65.
Table 1
Table 2
Table 3

Claims (5)

1. nonaqueous electrolytic solution the coupling that can further improve containing manganese high-temperature lithium ion battery impedance behavior has additive of stabilization function and uses thereof, it is characterized in that this electrolyte is comprised of four constituents: lithium salts, non-aqueous organic solvent, stabilization additives and other functional additives, this electrolyte is applied to manufacture the positive electrode active materials lithium ion battery to contain galaxite or to mix with nickle cobalt lithium manganate ternary phase.
2. according to claim 1 containing manganese electrolyte for lithium ion battery, it is characterized in that described lithium salts is one or more compositions that have in the compound of following molecular formula: LiPF 6, LiBF 4, LiBOB, LiClO 4, LiPF 3(C 2f 5) 3.
3. according to claim 1 can further improvement containing manganese high-temperature lithium ion battery impedance electrolyte, is characterized in that described stabilization additives is selected from any one above combination in three (trimethyl silane) phosphate, methane-disulfonic acid methylene ester, monoethanolamine.
4. according to claim 3ly can further improve the electrolyte of using containing the impedance of manganese high-temperature lithium ion battery, the addition that it is characterized in that described stabilization additives is 0.1%～5% of electrolyte total weight.
5. according to claim 1 can further improvement containing the purposes of electrolyte for the impedance of manganese high-temperature lithium ion battery, it is characterized in that described is the mixture of nickle cobalt lithium manganate ternary material and spinel lithium manganate containing manganese active material, and spinel lithium manganate weight accounts for 10%～100% of positive electrode active materials total weight.
CN201310135140.5A 2013-04-19 2013-04-19 Nonaqueous electrolyte additive capable of improving high-temperature impedance performance of manganese-contained lithium ion battery Pending CN104112869A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110994023A (en) * 2019-11-29 2020-04-10 湖北宇电能源科技股份有限公司 Lithium ion battery safety electrolyte, preparation method and application thereof, and lithium ion battery

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EP1050916A1 (en) * 1999-05-03 2000-11-08 Wilson Greatbatch Ltd. Phosphate additives for nonaqueous electrolyte in rechargeable electrochemical cells
CN101771167A (en) * 2010-02-05 2010-07-07 九江天赐高新材料有限公司 High-capacity lithium-ion electrolyte, battery and preparation method of battery
CN102263292A (en) * 2011-06-24 2011-11-30 九江天赐高新材料有限公司 Non-aqueous electrolytic solution used for lithium secondary batteries
CN102306835A (en) * 2011-09-02 2012-01-04 广州天赐高新材料股份有限公司 High voltage resistant and high temperature resistant safety type electrolyte for lithium ion battery adopting manganese material as anode, and use thereof
CN102324568A (en) * 2011-09-15 2012-01-18 诺莱特科技(苏州)有限公司 Electrolyte solution for improving swelling of lithium ion battery
CN102637901A (en) * 2012-04-24 2012-08-15 广州市云通磁电有限公司 Electrolyte for lithium ion battery and preparation method thereof
EP2498329A1 (en) * 2011-03-10 2012-09-12 SB LiMotive Co., Ltd. Non-aqueous electrolyte for rechargeable lithium battery and rechargeable lithium battery including the same
EP2503633A2 (en) * 2011-03-23 2012-09-26 SB LiMotive Co., Ltd. Electrolyte for rechargeable lithium battery and rechargeable lithium battery including the same

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1050916A1 (en) * 1999-05-03 2000-11-08 Wilson Greatbatch Ltd. Phosphate additives for nonaqueous electrolyte in rechargeable electrochemical cells
CN101771167A (en) * 2010-02-05 2010-07-07 九江天赐高新材料有限公司 High-capacity lithium-ion electrolyte, battery and preparation method of battery
EP2498329A1 (en) * 2011-03-10 2012-09-12 SB LiMotive Co., Ltd. Non-aqueous electrolyte for rechargeable lithium battery and rechargeable lithium battery including the same
EP2503633A2 (en) * 2011-03-23 2012-09-26 SB LiMotive Co., Ltd. Electrolyte for rechargeable lithium battery and rechargeable lithium battery including the same
CN102263292A (en) * 2011-06-24 2011-11-30 九江天赐高新材料有限公司 Non-aqueous electrolytic solution used for lithium secondary batteries
CN102306835A (en) * 2011-09-02 2012-01-04 广州天赐高新材料股份有限公司 High voltage resistant and high temperature resistant safety type electrolyte for lithium ion battery adopting manganese material as anode, and use thereof
CN102324568A (en) * 2011-09-15 2012-01-18 诺莱特科技(苏州)有限公司 Electrolyte solution for improving swelling of lithium ion battery
CN102637901A (en) * 2012-04-24 2012-08-15 广州市云通磁电有限公司 Electrolyte for lithium ion battery and preparation method thereof

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110994023A (en) * 2019-11-29 2020-04-10 湖北宇电能源科技股份有限公司 Lithium ion battery safety electrolyte, preparation method and application thereof, and lithium ion battery
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Inventor after: Shen Xiaoyan

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Application publication date: 20141022