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Solid electrolyte and all-solid-state battery

A solid electrolyte and micro-quantity technology, applied in secondary batteries, circuits, electrical components, etc., can solve problems affecting the quality of ceramic sheets, a large number of pores, shrinkage of ceramic sheets, and internal grain growth, etc., to improve and inhibit lithium dendrites Penetrating properties, high density, and stable cubic phase effects

Active Publication Date: 2019-05-31
BEIJING UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, due to high temperature sintering, the ceramic sheet shrinks and the internal grain grows abnormally, resulting in a large number of pores and grain boundaries, which seriously affect the quality of the ceramic sheet.

Method used

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  • Solid electrolyte and all-solid-state battery

Examples

Experimental program
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Effect test

Embodiment 1

[0039] Will Li 2 O, ZrO 2 , La 2 o 3 、WO 3 , CaO is proportioned according to the stoichiometric ratio Li:La:Ca:Zr:W=6.7:2.8:0.2:1.75:0.25. Before ball milling, the La 2 o 3 Dry at 900°C for 24h, Li 2 The excess of O is 5% to compensate for the loss of lithium during sintering. The raw materials were weighed and placed in a zirconia ball mill jar, and wet ball milled with absolute ethanol as the medium at a milling speed of 200 rpm for 15 hours. Dry the slurry to obtain a uniform powder, and then pre-fire the mixed powder at 900°C for 8h at a heating rate of 1°C / min to obtain 1.41% La 2 Zr 2 o 7 Solid electrolyte powder. In order to obtain a solid electrolyte with higher activity, the solid electrolyte powder is ball milled again. The process is the same as the above ball milling process, and the powder with a smaller particle size is obtained for tableting, and the powder is buried for sintering. The actual density of the solid electrolyte ceramic sheet is measure...

Embodiment 2

[0049] Will Li 2 O, ZrO 2 , La 2 o 3 、WO 3 , CaO is proportioned according to the stoichiometric ratio Li:La:Ca:Zr:W=6.6:2.9:0.1:1.75:0.25. Before ball milling, the La 2 o 3 Dry at 900°C for 24h, Li 2 The excess of O is 5% to compensate for the loss of lithium during sintering. The raw materials were weighed and placed in a zirconia ball mill jar, and wet ball milled with absolute ethanol as the medium at a milling speed of 200 rpm for 15 hours. Dry the slurry to obtain a uniformly mixed powder, and then pre-fire the mixed powder at 900°C for 8 hours at a heating rate of 1°C / min to obtain a trace La 2 Zr 2 o 7 Structured solid electrolyte powder. In order to obtain a solid electrolyte with higher activity, the solid electrolyte powder is ball milled again, and the process is the same as the above ball mill process to obtain a solid electrolyte powder with a smaller particle size. Image 6 It shows that the La-containing 2 Zr 2 o 7 Structure of the garnet-type so...

Embodiment 3

[0051] Will Li 2 O, ZrO 2 , La 2 o 3 、WO 3 , CaO is proportioned according to the stoichiometric ratio Li:La:Ca:Zr:W=6.6:2.9:0.1:1.75:0.25. Before ball milling, La 2 o 3 Dry at 900°C for 24h, Li 2 The excess of O is 5% to compensate for the loss of lithium during sintering. The raw materials were weighed and placed in a zirconia ball mill jar, and wet ball milled with absolute ethanol as the medium at a milling speed of 200 rpm for 15 hours. Dry the slurry to obtain a uniformly mixed powder, and then pre-fire the mixed powder at 900°C for 10h at a heating rate of 1°C / min to obtain a trace La 2 Zr 2 o 7 Structured solid electrolyte powder. In order to obtain a solid electrolyte with higher activity, the solid electrolyte powder is ball milled again, and the process is the same as the above ball milling process to obtain a solid electrolyte powder with a smaller particle size.

[0052] Figure 7 It shows that the La-containing 2 Zr 2 o 7 Structure of the garnet-t...

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Abstract

The invention relates to a solid electrolyte and an all-solid-state battery and belongs to the field of solid-state ion materials. A method comprises according to the nominal molar ratio of various elements in a garnet-type solid electrolyte chemical formula LiALaBMCNDZrEO12, subjecting a Li source, a La source, a Zr source, a M source, and an N source to wet ball milling and mixing; then providing 1 to 5% of excess Li source; drying and sieving the paste; and calcining uniformly mixed powder at high temperature under a certain condition to obtain a solid electrolyte material having a garnet-type cubic phase structure and containing a trace amount of La2Zr2O7 structure. A ceramic sheet prepared by using the solid electrolyte has high density, good ionic conductivity and good stability to lithium metal, and can be applied to solid-state lithium ion batteries.

Description

technical field [0001] The invention belongs to the field of solid-state ionic materials, and in particular relates to a 2 Zr 2 o 7 Structured garnet-type solid electrolyte material, its preparation method and application. Background technique [0002] Since lithium-ion batteries were commercialized in 1991, they have been widely used in portable electronic devices such as mobile phones and notebook computers. With the gradual increase in the safety requirements of national electric vehicles and large-scale energy storage grids, all-solid-state batteries are considered to reduce the occurrence of such safety hazards to a large extent and greatly improve the safe use performance of lithium batteries. In all-solid-state batteries, the solid-state electrolyte is the key, replacing the separator and electrolyte. At present, the electrolyte of lithium secondary batteries is mainly composed of organic solvents and lithium salts, and organic solvents have low boiling points, ar...

Claims

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Application Information

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IPC IPC(8): H01M10/0525H01M10/0562
CPCY02E60/10
Inventor 尉海军孙芙蓉王永涛郭现伟
Owner BEIJING UNIV OF TECH
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