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Method for fabrication of hybrid solid electrolyte membrane and all-solid-state lithium battery

A solid electrolyte membrane, composite technology, applied in non-aqueous electrolyte batteries, solid electrolytes, electrolytes, etc., can solve problems such as combustion, poor battery performance, and safety impact of lithium-ion batteries

Pending Publication Date: 2022-02-18
MING CHI UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, volatile and flammable liquid electrolytes have a great impact on the safety of lithium-ion batteries. After multiple charge / discharge cycles, in addition to the danger of overheating, combustion or even explosion, needle-shaped lithium branches are also prone to occur. The crystal causes problems such as internal short circuit of the battery
[0003] Although all-solid-state lithium batteries using solid-state electrolyte membranes can effectively avoid safety issues such as electrolyte leakage and combustion explosions, the growth of lithium dendrites and poor contact between solid-state electrolyte membranes and electrodes lead to excessively high interfacial impedance, and their / Lithium ion conductivity at room temperature (25°C) is generally low (about 10 -7 S cm -1 ) and other problems, resulting in poor overall battery performance
[0004] Therefore, for the lithium batteries of the prior art, how to avoid the growth of needle-like lithium dendrites, improve the conductivity of lithium ions, and reduce the interface impedance between the solid electrolyte membrane and the electrode, so that the battery has excellent performance, still needs to be improved. with promotion

Method used

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  • Method for fabrication of hybrid solid electrolyte membrane and all-solid-state lithium battery
  • Method for fabrication of hybrid solid electrolyte membrane and all-solid-state lithium battery
  • Method for fabrication of hybrid solid electrolyte membrane and all-solid-state lithium battery

Examples

Experimental program
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Effect test

Embodiment 1

[0069] "La 3 Zr 2 Ga 0.3 (OH) x,x=17.9 Hydroxide Precursor Preparation》

[0070] Compared with the traditional batch reactor (Batch reactor) preparation method, TFR produces a greater mixing force through the flow principle of Taylor fluid, which is about 7 times that of the traditional one, so it can be processed in a shorter reaction time (about 1 / 8 reaction time; faster mass transfer speed: 3.3vs.1.0m s -1 ) to obtain a smaller particle size distribution, about 1 / 2 the size of the traditional, pure cubic phase (Cubic phase) hydroxide precursor and high yield (reactor volume: 1 ~ 300L). Therefore, utilize TFR reactor to prepare La in the present invention 3 Zr 2 Ga 0.3 (OH) 17.9 , metal hydroxide precursors.

[0071] LaZrGa(OH) x One of the specific implementations of the preparation method of the metal hydroxide precursor is as follows:

[0072] First, weigh the metal salt powder to prepare 2M La(NO 3 ) 3 ·6H 2 O, ZrOCl 2 ·8H 2 O and Ga(NO 3 ) 3 The metal...

Embodiment 2

[0074] "Synthesis of ion-doped Ga-F-LLZO (i.e. Li 5.9 Ga 0.3 La 3 Zr 2 f 0.2 o 11.8 ) All-solid lithium ion conductive material》

[0075] The ion-doped Ga-F-LLZO all-solid-state lithium ion conductive material formed by fluorine doping (the metering is 0.2, using LiF as the ion doping source) is obtained by drying the La 3 Zr 2 Ga 0.3 (OH) 17.9 Metal hydroxide precursor, 10% excess LiOH.H 2 O (that is, the molar ratio is LaZrGa(OH) x : LiOH.H 2 O=1:6, in order to compensate for the subsequent loss of lithium in high temperature environment due to calcination heat treatment) and LiF is placed in a ball mill jar filled with 99% methanol solvent (using zirconia balls, the weight ratio of the mixture and the balls is 1:10), and through a planetary ball mill (Planetary Ball Mill PM 200, Retsch, Germany), the rotation speed is 400rpm, and the grinding and mixing time is about 20 minutes. After the grinding is completed, the grinding balls are first taken out of the ball...

Embodiment 3

[0079] "Preparation of Freestanding Double-layer Composite Solid Electrolyte (Bi-HSE) Membrane"

[0080] Independent double-layer composite solid electrolyte membrane, i.e. Ga-F-LLZO@PVDF+PAN / LiTFSI / SN / / Ga-F-LLZO@PVDF+PAN / LiTFSI / SN film of double-layer structure (in the present invention, The substances contained in the same layer of film are separated by / , and the different layers of film are separated by / / , and the position is arranged from top to bottom as "the first layer / / the second layer / / the third layer") One of the specific implementations of the method is as follows:

[0081] The independent double-layer composite solid electrolyte membrane with the function of conducting lithium ions is composed of polyvinylidene fluoride (PVDF) polymer, polyacrylonitrile (PAN) polymer, lithium bistrifluoromethanesulfonimide (LiTFSI) lithium salt , succinonitrile (SN) plasticizer and the ion-doped Ga-F-LLZO all-solid lithium ion conductive material of Example 2. During the pr...

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Abstract

The present invention provides a method for the fabrication of a LaZrGa(OH)x metal hydroxide precursor with a co-precipitation method in a continuous TFR reactor. The present invention also provides a method for the fabrication of an ion-doped all-solid-state lithium-ion conductive material with lithium ionic conductivity, and mixing which in the polymer base material, using a doctor-blade coating method to prepare a free standing double layered and triple layered organic-inorganic hybrid solid electrolyte membrane. Furthermore, the present invention provides an all-solid-state lithium battery using the aforementioned hybrid solid electrolyte membrane and measure the electrochemical performance. The all-solid-state lithium battery may enhance the lithium ionic conductivity, and lower the interfacial resistance between the solid electrolyte membrane and the electrode, therefore the battery may have excellent performance, and prevent the lithium-dendrite formation effectively to enhance the safety.

Description

technical field [0001] The present invention relates to a LaZrGa(OH) x A method for preparing a metal hydroxide precursor, a method for preparing an ion-doped all-solid lithium ion conducting material with lithium ion conductivity using the precursor, and a free standing (Free standing) using the all solid lithium ion conducting material ) double-layer and three-layer organic / inorganic composite solid electrolyte (Hybrid solid electrolyte, hereinafter also referred to as HSE) membrane preparation method, and apply the composite solid electrolyte membrane to an all-solid lithium battery. Background technique [0002] Lithium-ion batteries are often used in consumer electronics and transportation facilities due to their high open circuit voltage, high energy density, fast charge / discharge rate, long charge / discharge cycle life, low self-discharge, and light weight. power supply equipment. However, volatile and flammable liquid electrolytes have a great impact on the safety o...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M10/0562H01M10/0525H01M10/42
CPCH01M10/0562H01M10/0525H01M10/4235H01M10/052H01M10/056H01M2300/0082H01M2300/0071H01M2300/0094H01M4/382Y02E60/10H01M50/446H01M50/451H01M50/403
Inventor 杨纯诚吴宜萱库姆拉切夫·泽拉勒姆·瓦勒
Owner MING CHI UNIVERSITY OF TECHNOLOGY
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