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Solid electrolyte and preparation method thereof, solid battery and electronic equipment

A solid electrolyte and electrolyte technology, applied in the field of lithium-ion batteries, can solve problems affecting battery energy density, reduce ionic conductivity, and mechanical strength lithium metal compatibility issues, and achieve excellent charge and discharge characteristics, good electrochemical stability, The effect of good cycle performance

Inactive Publication Date: 2019-10-15
BEIJING INST OF COLLABORATIVE INNOVATION
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Problems solved by technology

In the prior art, the ceramic-based composite solid-state electrolyte prepared by mixing ceramic powder and organic polymer filler has obtained flexibility to a certain extent and improved the contact interface between the electrolyte and the lithium negative electrode, but the ionic conductivity has decreased significantly. , the particles are easy to agglomerate and hinder the transmission of lithium ions; the ceramic-based composite solid-state electrolyte prepared by using the method of modifying the interface with lithium-conducting organic substances on the surface of the inorganic ceramic sheet, although it takes advantage of the ionic conductivity of the inorganic electrolyte, it is also optimized to a certain extent. The interface performance is improved, but the electrolyte is thick, brittle, and not flexible. At the same time, the organic lithium-conducting interface layer will reduce the overall ionic conductivity and affect the overall energy density of the battery.
[0003] Patent documents CN109075384A, CN107394255A, CN103151557A, CN108963327A and CN106935903A all use inorganic materials as fillers, or prepare polymer-based composite solid electrolytes with polymer matrix as the main body, or prepare gel-based composite electrolytes with gel as the matrix. The electrical conductivity, thermal stability, and electrochemical stability have been improved, but the overall electrical conductivity is still low, and the application at room temperature is hindered. The latter has more serious safety issues, mechanical strength issues, and compatibility with lithium metal. sexual problems
[0004] Patent documents CN107369848A, CN107452983A, and CN108336402A use inorganic solid-state electrolytes as substrates to better utilize the advantages of inorganic lithium-conducting materials, and to a certain extent improve the problems of composite electrolytes and lithium negative electrodes, but have poor flexibility, insufficient mechanical properties, or poor preparation processes. Complicated, unable to effectively solve the interface problem with the lithium negative electrode
[0005] It can be seen that the prior art lacks solid electrolytes with good flexibility, high ionic conductivity, good electrochemical stability, and good interface stability.

Method used

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preparation example Construction

[0064] According to the second aspect of the present invention, the embodiment of the present invention proposes a method for preparing a flexible ceramic matrix composite solid electrolyte, including the following steps:

[0065] S1. Preparation of inorganic solid electrolyte ceramic matrix

[0066] Mix materials containing inorganic solid electrolyte and binder; grind for 1-4 hours; apply 0.1Mpa-10MPa pressure;

[0067] S2. Filling with organic additives and lithium salts with lithium-conducting ability

[0068] Mixing the organic additive with lithium conduction ability and lithium salt; preparing the mixture containing the organic additive with lithium conduction ability and lithium salt into a liquid mixture; immersing the inorganic solid electrolyte ceramic matrix obtained in step S1 into the liquid mixture.

[0069] The preparation of the mixture containing the organic additive with the ability to conduct lithium and the lithium salt into a liquid mixture is, for examp...

Embodiment 1

[0072] S1. Preparation of ceramic matrix

[0073] In an argon glove box, the binder polytetrafluoroethylene (PTFE) and the inorganic solid electrolyte Li 7 La 3 Zr 2 o 12 (LLZO) was thoroughly mixed at a mass ratio of 5:95, and ground for 1 hour to obtain a rough embryo of ceramic matrix film. The particle size range of the ground material was 0.1 μm-10 μm; The rough membrane is provided with a pressure of 3 MPa, and the pressure is maintained for 30 minutes to prepare a uniform ceramic matrix membrane.

[0074] S2. Filling with organic additives and lithium salts with lithium-conducting ability

[0075] Mix the organic additive succinonitrile (SN) with lithium-conducting ability and the lithium salt LiTFSI at a mass ratio of 4:1, then heat the mixture to 80°C and melt it into a liquid state to form a liquid mixture; immerse the ceramic substrate obtained in step S1 into the above-mentioned After 48 hours in the liquid mixture, take it out, let it stand to remove the resi...

Embodiment 2

[0079] S1. Preparation of ceramic matrix

[0080] In an argon glove box, the binder polytetrafluoroethylene (PTFE) and the inorganic solid electrolyte Li 10 GeP 2 S 12 After fully mixing at a mass ratio of 5:90, grind for 1 hour to obtain a rough ceramic matrix membrane. The particle size of the ground material ranges from 0.1 μm to 10 μm; Provide a pressure of 1 MPa and keep the pressure for 30 minutes to prepare a uniform ceramic matrix film.

[0081] S2. Filling with organic additives and lithium salts with lithium-conducting ability

[0082] The organic additive 1,2-diethyl-3-methylimidazolium trifluoromethanesulfonate (C 7 h 11 f 3 N 2 o 3 S) mix with lithium salt LiFSI at a mass ratio of 5:1, the organic additive dissolves LiFSI to form a solution; immerse the ceramic matrix obtained in step S1 in the above solution for 48 hours, take it out, and let it stand to remove the residue to obtain a flexible ceramic matrix composite solid electrolyte. Among them, PTFE...

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Abstract

The embodiment of the invention relates to a flexible ceramic matrix composite solid electrolyte and a preparation method thereof, a solid battery and electronic equipment. The flexible ceramic matrixcomposite solid electrolyte comprises an inorganic solid electrolyte ceramic matrix and an organic additive having a lithium conducing capability and lithium salt. The inorganic solid electrolyte ceramic matrix is prepared by utilizing a material containing an inorganic solid electrolyte and a binder by adopting a dry method; the organic additive with the lithium conducting capability and the lithium salt are filled in the inorganic solid electrolyte ceramic matrix. The flexible ceramic matrix composite solid electrolyte has good flexibility, high ionic conductivity, good electrochemical stability and good interface stability.

Description

technical field [0001] The invention belongs to the technical field of lithium-ion batteries, and in particular relates to a flexible ceramic-based composite solid electrolyte and a preparation method thereof, a flexible solid-state battery and electronic equipment. Background technique [0002] Ceramic-based composite electrolytes are currently a hot spot in the development of solid-state batteries. In the prior art, the ceramic-based composite solid-state electrolyte prepared by mixing ceramic powder and organic polymer filler has obtained flexibility to a certain extent and improved the contact interface between the electrolyte and the lithium negative electrode, but the ionic conductivity has decreased significantly. , the particles are easy to agglomerate and hinder the transmission of lithium ions; the ceramic-based composite solid-state electrolyte prepared by using the method of modifying the interface with lithium-conducting organic substances on the surface of the ...

Claims

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Application Information

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IPC IPC(8): H01M10/0562H01M10/0564H01M10/0565H01M10/0525
CPCH01M10/0525H01M10/0562H01M10/0564H01M10/0565H01M2300/0065H01M2300/0091Y02E60/10
Inventor 范丽珍蒋涛立陈龙
Owner BEIJING INST OF COLLABORATIVE INNOVATION
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