CN105470564A - Solid electrolyte membrane, preparation method of solid electrolyte membrane and lithium ion battery - Google Patents

Solid electrolyte membrane, preparation method of solid electrolyte membrane and lithium ion battery Download PDF

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Publication number
CN105470564A
CN105470564A CN201610061128.8A CN201610061128A CN105470564A CN 105470564 A CN105470564 A CN 105470564A CN 201610061128 A CN201610061128 A CN 201610061128A CN 105470564 A CN105470564 A CN 105470564A
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China
Prior art keywords
ion battery
lithium ion
solid electrolyte
glass ceramic
electrolyte membrane
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Pending
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CN201610061128.8A
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Chinese (zh)
Inventor
王群峰
谷秀娟
董苗苗
梁振洋
吴楚伟
叶付臣
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SHANDONG HONGZHENG BATTERY MATERIAL TECHNOLOGY Co Ltd
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SHANDONG HONGZHENG BATTERY MATERIAL TECHNOLOGY Co Ltd
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Priority to CN201610061128.8A priority Critical patent/CN105470564A/en
Publication of CN105470564A publication Critical patent/CN105470564A/en
Pending legal-status Critical Current

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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
    • 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
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • 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 invention discloses a solid electrolyte membrane of a lithium ion battery, and relates to the field of lithium ion batteries. The solid electrolyte membrane is composed of a glass ceramic electrolyte and a coating layer with which the surface of the glass ceramic electrolyte is coated. The coating layer is prepared from lithium salt and a polymer material at the molar ratio of 1:5-1:10. The electrolyte membrane can reduce the interface impedance of the full-solid-state lithium ion battery to a great extent, so that the cycling stability of the full-solid-state lithium ion battery is improved, and the service life of the full-solid-state lithium ion battery is prolonged. The invention further discloses a preparation method of the solid electrolyte membrane and the full-solid-state lithium ion battery comprising the solid electrolyte membrane. The solid electrolyte membrane of the lithium ion battery is high in mechanical strength and excellent in electrochemical performance, and meanwhile the preparation technology is simple and convenient to popularize.

Description

A kind of solid electrolyte film and preparation method thereof and lithium ion battery
Technical field:
The present invention is specifically related to a kind of solid electrolyte film and preparation method thereof and the solid Li-ion battery containing this dielectric film.
Background technology:
From the nineties in 20th century first piece of commercial applications lithium ion battery be born since, the advantages such as lithium ion battery is high with its energy density, power output large, memory-less effect, are used widely in fields such as PC, mobile electronic device, electric automobile, electric tool, energy storage devices.Along with the progress of technology, every chemical property such as energy density, the cycle performance etc. of lithium ion battery are also obtained for great lifting.But because current lithium ion battery still widely uses liquid state organic electrolyte, its safety high is not still solved at all.
Different from conventional lithium ion battery, solid lithium ion battery, due to not containing liquid organic solvent, fundamentally can stop the risk of cells burst blast.Thus, for the mankind provide one new type lithium ion battery safely and effectively.But, in miscellaneous solid electrolyte, inorganic sulfenyl glass ceramic electrolyte closest to practical level very easily reacts with the power and water pole active material of trace and decomposes, form higher Ion transfer impedance in the interface of solid electrolyte and electrode material, thus have a strong impact on every chemical property of solid Li-ion battery.
Summary of the invention:
In view of this, first aspect present invention provides a kind of solid electrolyte film that significantly can reduce above-mentioned interface impedance.By coated method, one coating layer is set on glass ceramic electrolyte surface, thus forms a transition zone at solid electrolyte and electrode material interface, reduce interface ion migration impedance.Second aspect present invention provides the preparation method of this solid electrolyte membrane.Third aspect present invention provides the solid Li-ion battery containing this solid electrolyte film.
First aspect, the invention provides a kind of lithium ion battery solid electrolyte film, and comprise glass ceramic electrolyte and the coating layer being coated on its surface, described coating layer material comprises lithium salts and the polymeric material of mol ratio 1: 5 ~ 1: 10.Wherein, described glass ceramic electrolyte is Li 2s-P 2s 5with Li 10geP 2s 12in at least one; Described lithium salts be in LiTFSI and LiFSI at least; Described polymer is at least one in PEO, PAN, PMMA, PVDF.
Second aspect, the invention provides a kind of preparation method of lithium ion battery solid electrolyte film, it is characterized in that, comprise the following steps:
(1) getting appropriate glass ceramic electrolyte powder is dispersed in anhydrous toluene solution, is then uniformly coated on aramid fiber nonwoven fabrics with scraper, fully dry in inert environments.
(2) the dried nonwoven fabrics being coated with glass ceramic electrolyte is colded pressing, obtain glass ceramic electrolyte/nonwoven fabrics diaphragm.
(3) getting appropriate polymer beads is dissolved in anhydrous acetonitrile, then adds appropriate lithium salts, and ultrasonic process is dissolved completely to polymer and lithium salts, and the mol ratio of lithium salts and polymer controls between 1: 5 ~ 1: 10.
(4) step (3) gained solution is evenly arranged on step (2) gained glass ceramic electrolyte/nonwoven fabrics diaphragm by method of electrostatic spinning or liquid phase spraying process, in inert atmosphere, after drying, both obtained lithium ion battery solid electrolyte membrane.
Wherein, in described step (1), aramid fiber nonwoven fabrics material is PPTA, porosity ~ 70%, aperture ~ 30 μm.
The third aspect, the invention provides a kind of solid Li-ion battery, the solid electrolyte film comprising positive pole, negative pole and be placed between both positive and negative polarity.Preparation process is as follows: positive pole, solid electrolyte membrane, negative pole are obtained nude battery core by lamination process, battery core is encapsulated with aluminum plastic film, after changing into, obtain solid Li-ion battery.
Lithium ion battery solid electrolyte film mechanical strength of the present invention is high, electrochemical performance, and meanwhile, preparation technology is simple, is convenient to promote.
Embodiment:
For illustrating this aspect further, describe the preferred embodiments of the invention below in conjunction with specific embodiment, these describe just in order to further illustrate advantage of the present invention, instead of limiting to the claimed invention.
Embodiment 1
A preparation method for lithium ion battery solid electrolyte film, comprises the following steps:
(1) appropriate glass ceramic electrolyte powder Li is got 2s-P 2s 5be dispersed in anhydrous toluene solution, be then uniformly coated on aramid fiber nonwoven fabrics with scraper, fully dry in inert environments.
(2) the dried nonwoven fabrics being coated with glass ceramic electrolyte is colded pressing, obtain Li 2s-P 2s 5/ nonwoven fabrics diaphragm.
(3) getting appropriate PEO is dissolved in anhydrous acetonitrile, then adds appropriate LiTFSI, and ultrasonic process is dissolved completely to PEO and LiTFSI, and the mol ratio of PEO and LiTFSI is 1: 7.
(4) step (3) gained solution is evenly arranged on step (2) gained Li by method of electrostatic spinning 2s-P 2s 5on/nonwoven fabrics diaphragm, in inert atmosphere, after drying, both obtained lithium ion battery solid electrolyte membrane M1.
A preparation method for solid Li-ion battery, comprises the following steps:
(1) take LiCoO2 as positive electrode, add bonding agent Kynoar (PVDF), conductive agent conductive black is sized mixing in 1-methyl-9-pyrrolidinone solvent, gained slurry double-faced uniform is coated on aluminium foil, drying, roll extrusion, obtains anode pole piece after cutting.
(2) take graphite as negative material, add butadiene-styrene rubber (SBR), sodium carboxymethylcellulose (CMC), graphite sizes mixing in deionized water, gained slurry double-faced uniform is coated on Copper Foil, drying, roll extrusion, obtains cathode pole piece after cutting.
(3) anode pole piece, solid electrolyte film M1, cathode pole piece are done battery core by lamination process is obtained, be placed in baking oven with aluminum plastic film encapsulation and toast.Through shaping, change into after experimental solids lithium ion battery.
Embodiment 2
A preparation method for lithium ion battery solid electrolyte film, comprises the following steps:
(1) appropriate glass ceramic electrolyte powder Li is got 2s-P 2s 5be dispersed in anhydrous toluene solution, be then uniformly coated on aramid fiber nonwoven fabrics with scraper, fully dry in inert environments.
(2) the dried nonwoven fabrics being coated with glass ceramic electrolyte is colded pressing, obtain Li 2s-P 2s 5/ nonwoven fabrics diaphragm.
(3) getting appropriate PMMA is dissolved in anhydrous acetonitrile, then adds appropriate LiFSI, and ultrasonic process is dissolved completely to PMMA and LiFSI, and the mol ratio of PMMA and LiFSI is 1: 8.
(4) step (3) gained solution is evenly arranged on step (2) gained Li by method of electrostatic spinning 2s-P 2s 5on/nonwoven fabrics diaphragm, in inert atmosphere, after drying, both obtained lithium ion battery solid electrolyte membrane M2.
As described in Example 1, difference is only the lithium ion battery solid electrolyte membrane M2 using the present embodiment obtained to a kind of preparation method of solid Li-ion battery.
Embodiment 3
A preparation method for lithium ion battery solid electrolyte film, comprises the following steps:
(1) appropriate glass ceramic electrolyte powder Li is got 10geP 2s 12be dispersed in anhydrous toluene solution, be then uniformly coated on aramid fiber nonwoven fabrics with scraper, fully dry in inert environments.
(2) the dried nonwoven fabrics being coated with glass ceramic electrolyte is colded pressing, obtain Li 10geP 2s 12/ nonwoven fabrics diaphragm.
(3) getting appropriate PEO is dissolved in anhydrous acetonitrile, then adds appropriate LiTFSI, and ultrasonic process is dissolved completely to PEO and LiTFSI, and the mol ratio of PEO and LiTFSI is 1: 7.
(4) step (3) gained solution is evenly arranged on step (2) gained Li by liquid phase spraying process 10geP 2s 12on/nonwoven fabrics diaphragm, in inert atmosphere, after drying, both obtained lithium ion battery solid electrolyte membrane M3.
As described in Example 1, difference is only the lithium ion battery solid electrolyte membrane M3 using the present embodiment obtained to a kind of preparation method of solid Li-ion battery.
Comparative example 1
As described in Example 1, difference is only the Li obtained by preparation method's step 2 using a kind of lithium ion battery solid electrolyte film in embodiment 1 to a kind of preparation method of solid Li-ion battery 2s-P 2s 5/ nonwoven fabrics diaphragm is solid electrolyte membrane.
Effect detects:
By the experimental cell in comparative example 1 and embodiment 1 in the voltage range of 3.0 ~ 4.35V, carry out 0.5C discharge and recharge 600 weeks loop tests.In test result display embodiment 1, after experimental cell circulation, capability retention is 89%, and the capability retention of comparative example 1 experimental cell is 81%.As can be seen here, lithium ion battery solid electrolyte provided by the invention obviously can improve the performance of solid Li-ion battery.

Claims (7)

1. a lithium ion battery solid electrolyte film, is characterized in that, comprise glass ceramic electrolyte and the coating layer being coated on its surface, described coating layer material comprises lithium salts and the polymeric material of mol ratio 1: 5 ~ 1: 10.
2. a kind of lithium ion battery solid electrolyte film according to claim 1, is characterized in that, described glass ceramic electrolyte is Li 2s-P 2s 5with Li 10geP 2s 12in at least one.
3. a kind of lithium ion battery solid electrolyte film according to claim 1, is characterized in that, described lithium salts is at least one in LiTFSI and LiFSI.
4. a kind of lithium ion battery solid electrolyte film according to claim 1, is characterized in that, described polymer is at least one in PEO, PAN, PMMA, PVDF.
5. a preparation method for lithium ion battery solid electrolyte film, is characterized in that, comprises the following steps:
(1) getting appropriate glass ceramic electrolyte powder is dispersed in anhydrous toluene solution, is then uniformly coated on aramid fiber nonwoven fabrics with scraper, fully dry in inert environments;
(2) the dried nonwoven fabrics being coated with glass ceramic electrolyte is colded pressing, obtain glass ceramic electrolyte/nonwoven fabrics diaphragm;
(3) getting appropriate polymer beads is dissolved in anhydrous acetonitrile, then adds appropriate lithium salts, and ultrasonic process is dissolved completely to polymer and lithium salts, and the mol ratio of lithium salts and polymer controls between 1: 5 ~ 1: 10;
(4) step (3) gained solution is evenly arranged on step (2) gained glass ceramic electrolyte/nonwoven fabrics diaphragm by method of electrostatic spinning or liquid phase spraying process, in inert atmosphere, after drying, both obtained lithium ion battery solid electrolyte membrane.
6. the preparation method of a kind of lithium ion battery solid electrolyte film according to claim 5, is characterized in that, in described step (1), aramid fiber nonwoven fabrics material is PPTA, porosity ~ 70%, aperture ~ 30 μm.
7. a solid Li-ion battery, is characterized in that, comprises positive pole, negative pole and is placed on the solid electrolyte film as claimed in claim 1 between both positive and negative polarity.
CN201610061128.8A 2016-01-22 2016-01-22 Solid electrolyte membrane, preparation method of solid electrolyte membrane and lithium ion battery Pending CN105470564A (en)

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Cited By (17)

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CN106654362A (en) * 2016-12-07 2017-05-10 珠海光宇电池有限公司 Composite solid electrolyte membrane, preparation method and lithium-ion battery
CN107195962A (en) * 2017-06-19 2017-09-22 宁波力赛康新材料科技有限公司 A kind of composite solid electrolyte and preparation method thereof
CN107452983A (en) * 2016-05-31 2017-12-08 比亚迪股份有限公司 A kind of lithium ion battery composite electrolyte and preparation method thereof and lithium ion battery
CN107978789A (en) * 2017-11-26 2018-05-01 中国科学院青岛生物能源与过程研究所 A kind of sulfide composite electrolyte of polymer conductive fibre toughness reinforcing
CN108206300A (en) * 2016-12-16 2018-06-26 现代自动车株式会社 Low-porosity solid electrolyte film and its manufacturing method
CN108539261A (en) * 2018-04-12 2018-09-14 上海空间电源研究所 A kind of high stable solid electrolyte preparation method of surface deposition inorganic salts
CN109167090A (en) * 2018-08-28 2019-01-08 长沙矿冶研究院有限责任公司 A kind of film build method of polymer-based solid state electrolyte
CN109786817A (en) * 2019-01-23 2019-05-21 蜂巢能源科技有限公司 Solid state lithium battery and its application and the method for preparing the solid electrolyte membrane that non-woven fabrics enhances
CN110034330A (en) * 2019-04-10 2019-07-19 华北电力大学 A kind of preparation method of lithium/sode cell composite solid electrolyte
CN110192302A (en) * 2017-05-15 2019-08-30 株式会社Lg化学 The manufacturing method of all-solid-state battery solid electrolyte film and the solid electrolyte film manufactured by the method
CN110957525A (en) * 2018-09-27 2020-04-03 比亚迪股份有限公司 Solid electrolyte, preparation method thereof and solid lithium battery
CN111106380A (en) * 2019-12-30 2020-05-05 华南师范大学 Preparation method of solid electrolyte with surface coating and solid electrolyte battery
CN111653820A (en) * 2018-02-11 2020-09-11 中国科学院苏州纳米技术与纳米仿生研究所 Solid electrolyte and application thereof
CN111933999A (en) * 2020-09-15 2020-11-13 江苏时代新能源科技有限公司 Solid-state battery, battery module, battery pack and related device thereof
CN112687946A (en) * 2020-12-23 2021-04-20 北京理工大学前沿技术研究院 Method for preparing functional inorganic solid electrolyte powder by vacuum coating technology
CN113782824A (en) * 2021-08-20 2021-12-10 蜂巢能源科技有限公司 Sulfide electrolyte membrane and preparation method and application thereof
WO2022166937A1 (en) * 2021-02-02 2022-08-11 Microvast Power Systems Co., Ltd. Solid state electrolyte and lithium-ion battery including solid state electrolyte

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CN107452983B (en) * 2016-05-31 2020-05-22 比亚迪股份有限公司 Lithium ion battery composite electrolyte, preparation method thereof and lithium ion battery
CN107452983A (en) * 2016-05-31 2017-12-08 比亚迪股份有限公司 A kind of lithium ion battery composite electrolyte and preparation method thereof and lithium ion battery
CN106654362A (en) * 2016-12-07 2017-05-10 珠海光宇电池有限公司 Composite solid electrolyte membrane, preparation method and lithium-ion battery
CN106654362B (en) * 2016-12-07 2019-07-19 珠海光宇电池有限公司 Composite solid electrolyte film, preparation method and lithium ion battery
CN108206300A (en) * 2016-12-16 2018-06-26 现代自动车株式会社 Low-porosity solid electrolyte film and its manufacturing method
US11335951B2 (en) 2016-12-16 2022-05-17 Hyundai Motor Company Low porosity solid electrolyte membrane and method for manufacturing the same
US11908993B2 (en) 2017-05-15 2024-02-20 Lg Energy Solution, Ltd. Method for manufacturing solid electrolyte membrane for all solid type battery and solid electrolyte membrane manufactured by the method
US11342578B2 (en) 2017-05-15 2022-05-24 Lg Energy Solution, Ltd. Method for manufacturing solid electrolyte membrane for all solid type battery and solid electrolyte membrane manufactured by the method
CN110192302A (en) * 2017-05-15 2019-08-30 株式会社Lg化学 The manufacturing method of all-solid-state battery solid electrolyte film and the solid electrolyte film manufactured by the method
CN110192302B (en) * 2017-05-15 2022-09-13 株式会社Lg新能源 Method for manufacturing solid electrolyte membrane for all-solid battery and solid electrolyte membrane manufactured by the method
CN107195962A (en) * 2017-06-19 2017-09-22 宁波力赛康新材料科技有限公司 A kind of composite solid electrolyte and preparation method thereof
CN107978789A (en) * 2017-11-26 2018-05-01 中国科学院青岛生物能源与过程研究所 A kind of sulfide composite electrolyte of polymer conductive fibre toughness reinforcing
CN107978789B (en) * 2017-11-26 2020-07-14 中国科学院青岛生物能源与过程研究所 Polymer conductive fiber toughened sulfide composite electrolyte
CN111653820A (en) * 2018-02-11 2020-09-11 中国科学院苏州纳米技术与纳米仿生研究所 Solid electrolyte and application thereof
CN108539261B (en) * 2018-04-12 2021-01-26 上海空间电源研究所 Preparation method of high-stability solid electrolyte with inorganic salt deposited on surface
CN108539261A (en) * 2018-04-12 2018-09-14 上海空间电源研究所 A kind of high stable solid electrolyte preparation method of surface deposition inorganic salts
CN109167090B (en) * 2018-08-28 2021-10-15 长沙矿冶研究院有限责任公司 Film forming method of polymer-based solid electrolyte
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CN110957525A (en) * 2018-09-27 2020-04-03 比亚迪股份有限公司 Solid electrolyte, preparation method thereof and solid lithium battery
CN110957525B (en) * 2018-09-27 2021-04-20 比亚迪股份有限公司 Solid electrolyte, preparation method thereof and solid lithium battery
CN109786817A (en) * 2019-01-23 2019-05-21 蜂巢能源科技有限公司 Solid state lithium battery and its application and the method for preparing the solid electrolyte membrane that non-woven fabrics enhances
CN109786817B (en) * 2019-01-23 2021-09-21 蜂巢能源科技有限公司 Solid lithium battery, application thereof and method for preparing non-woven fabric reinforced solid electrolyte membrane
CN110034330A (en) * 2019-04-10 2019-07-19 华北电力大学 A kind of preparation method of lithium/sode cell composite solid electrolyte
CN111106380A (en) * 2019-12-30 2020-05-05 华南师范大学 Preparation method of solid electrolyte with surface coating and solid electrolyte battery
CN111933999B (en) * 2020-09-15 2021-03-26 江苏时代新能源科技有限公司 Solid-state battery, battery module, battery pack and related device thereof
CN111933999A (en) * 2020-09-15 2020-11-13 江苏时代新能源科技有限公司 Solid-state battery, battery module, battery pack and related device thereof
CN112687946A (en) * 2020-12-23 2021-04-20 北京理工大学前沿技术研究院 Method for preparing functional inorganic solid electrolyte powder by vacuum coating technology
CN112687946B (en) * 2020-12-23 2022-01-07 北京理工大学前沿技术研究院 Method for preparing functional inorganic solid electrolyte powder by vacuum coating technology
WO2022166937A1 (en) * 2021-02-02 2022-08-11 Microvast Power Systems Co., Ltd. Solid state electrolyte and lithium-ion battery including solid state electrolyte
CN113782824A (en) * 2021-08-20 2021-12-10 蜂巢能源科技有限公司 Sulfide electrolyte membrane and preparation method and application thereof

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Application publication date: 20160406