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Method for improving compactness and conductivity of tantalum-doped garnet type solid electrolyte

A solid-state electrolyte, garnet-type technology, applied in the field of electrochemical energy storage, can solve the problems of insufficient electrical conductivity and density, and achieve the effects of improving cycle stability, low sintering cost, and eliminating hole defects.

Active Publication Date: 2021-09-17
HARBIN INST OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0008] The present invention solves the technical problem that the electrical conductivity and density of the existing tantalum-doped garnet-type solid electrolyte have not been fully improved; and provides a method for improving the density and electrical conductivity of the tantalum-doped garnet-type solid electrolyte

Method used

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  • Method for improving compactness and conductivity of tantalum-doped garnet type solid electrolyte
  • Method for improving compactness and conductivity of tantalum-doped garnet type solid electrolyte
  • Method for improving compactness and conductivity of tantalum-doped garnet type solid electrolyte

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Embodiment 1

[0038] A method for improving the density and conductivity of the tantalum-doped garnet-type solid electrolyte of the present embodiment adopts the tantalum-doped garnet-type solid-state electrolyte as Li 2 CO 3 , La 2 o 3 , ZrO 2 and Ta 2 o 5 The mixed powder is solid-phase sintered, and the sintering process is obtained by adding La 2 o 3 Nanoparticles to mediate mesophase La 2 Zr 2 o 7 (LaTaO 4 ), which in turn promotes the formation of LLZTO at grain boundaries. Specifically, it is accomplished through the following steps:

[0039] Step 1. According to Li 6.5 La 3 Zr 1.5 Ta 0.5 o 12 Weigh Li 2 CO 3 , La 2 o 3 , ZrO 2 and Ta 2 o 5 Mix well after powder, Li 2 CO 3 Excessive 10wt.%, use isopropanol to carry out wet ball milling as solvent, the volume of isopropanol and the mass ratio of mixed powder are 70ml:20g, and the grinding ball is the ZrO that diameter is 4mm and 6mm 2 Balls, the mass ratio of the two balls is 1:1, the mass ratio of the mixed ...

Embodiment 2

[0046] A method for improving the density and conductivity of the tantalum-doped garnet-type solid electrolyte of the present embodiment adopts the tantalum-doped garnet-type solid-state electrolyte as Li 2 CO 3 , La 2 o 3 , ZrO 2 and Ta 2 o 5 The mixed powder is solid-phase sintered, and the sintering process is obtained by adding La 2 o 3 Nanoparticles to mediate mesophase La 2 Zr 2 o 7 (LaTaO 4 ), which in turn promotes the formation of LLZTO at grain boundaries. Specifically, it is accomplished through the following steps:

[0047] Step 1. According to Li 6.5 La 3 Zr 1.5 Ta 0.5 o 12 Weigh Li 2 CO 3 , La 2 o 3 , ZrO 2 and Ta 2 o 5 Mix well after powder, Li 2 CO 3 Excess 10wt.%, La 2 o 3 Excessive 5wt.%, use isopropanol to carry out wet ball milling as solvent, the volume of isopropanol and mixed powder mass ratio are 70ml: 20g, and grinding ball is the ZrO that diameter is 4mm and 6mm 2 Balls, the mass ratio of the two types of balls is 1:1, the ...

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Abstract

The invention discloses a method for improving compactness and conductivity of tantalum-doped garnet type solid electrolyte, and belongs to the field of electrochemical energy storage. The invention aims to solve the technical problem that the conductivity and compactness of the existing tantalum garnet-doped solid electrolyte are not fully improved. The method comprises the steps of powder mixing, wet ball milling, drying, presintering, wet ball milling, drying, grinding and sieving, glue mixing and tabletting, degumming, and powder burying and sintering. According to the tantalum-doped garnet type solid electrolyte and the preparation method thereof, the element proportion of the La site and the Zr (Ta) site in the tantalum-doped garnet type solid electrolyte LLTZO is adjusted by doping La2O3 nano-particles, then generation of an intermediate phase LaTaO4 is mediated, abnormal grain growth of the LLTZO is effectively inhibited, the sintering homogeneity of the tantalum-doped garnet type solid electrolyte is improved, meanwhile, hole defects are reduced or eliminated to improve the compactness, therefore, the ionic conductivity is improved, and the cycling stability of the solid-state battery is improved. The method is simple, the sintering cost is low, and industrial mass production is easy to realize.

Description

technical field [0001] The invention belongs to the field of electrochemical energy storage; in particular, it relates to a method for improving the density and conductivity of a tantalum-doped garnet-type solid electrolyte. Background technique [0002] With the rapid development of lithium-ion batteries, higher requirements are placed on the safety of batteries, and the discovery of solid-state electrolytes can meet this requirement. Garnet-type solid electrolyte (Li 7 La 3 Zr 2 o 12 ) is one of the electrolytes with the most development potential, but the low conductivity and density are urgent problems to be solved. [0003] At present, more lithium ion vacancies can be provided by element doping, the cubic phase can be stabilized, the sintering temperature can be reduced and the fluidity of the liquid phase can be reduced, thereby improving the density and electrical conductivity. Among them, the doping of tantalum can effectively improve the The conductivity of th...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C04B35/48C04B35/50C04B35/622H01M10/0562H01M10/0525
CPCC04B35/48C04B35/50C04B35/622H01M10/0562H01M10/0525H01M2300/0071C04B2235/3203C04B2235/3227C04B2235/3248C04B2235/3255C04B2235/77C04B2235/96C04B2235/5454Y02E60/10
Inventor 黄永宪秦志伟孟祥晨万龙
Owner HARBIN INST OF TECH
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