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Lithium-lanthanum-zirconium oxide-based solid electrolyte material with stable surface, and preparation method and application thereof

A technology of solid electrolyte, lithium lanthanum zirconium oxide, applied in the manufacture of electrolyte batteries, electrolytes, non-aqueous electrolyte batteries, etc., can solve the problems of reduced ionic conductivity, large solid electrolyte/electrode interface impedance, safety restrictions on lithium-ion batteries, etc. , to achieve the effects of improving chemical stability, improving energy density and cycle stability, and broadening the application range

Active Publication Date: 2019-08-27
济宁克莱泰格新能源科技有限公司
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, safety issues have always been a major bottleneck restricting the application of lithium-ion batteries in large-scale energy storage fields such as power batteries and smart grids.
Both surface lithium carbonate and proton exchange reactions lead to a decrease in the ionic conductivity of LLZO
In addition, the researchers found that LLZO with lithium carbonate on the surface is used in solid-state lithium batteries, and the solid electrolyte / electrode interface impedance is large and the interface stability is poor.

Method used

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  • Lithium-lanthanum-zirconium oxide-based solid electrolyte material with stable surface, and preparation method and application thereof
  • Lithium-lanthanum-zirconium oxide-based solid electrolyte material with stable surface, and preparation method and application thereof
  • Lithium-lanthanum-zirconium oxide-based solid electrolyte material with stable surface, and preparation method and application thereof

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preparation example Construction

[0040] The preparation method of the lithium lanthanum zirconium oxide solid electrolyte material with stable surface comprises:

[0041] (1) Preparation of the lithium lanthanum zirconium oxide solid electrolyte (LLZO);

[0042] The preparation method of lithium lanthanum zirconium oxide solid electrolyte (LLZO) is a sol-gel method, and the preparation steps include: the precursors of lithium Li, lanthanum La, zirconium Zr and doping element M are prepared according to the formula of Li, La, Zr, M The molar ratio is (5+x): 3:x:(2-x) mixing, adding a solvent to dissolve, adding a chelating agent to form a sol-gel, heating and evaporating the solvent to obtain a mixed powder; grinding the mixed powder, first in Sintering at 250-600° C. for 2-48 hours, grinding again, and sintering at 500-1000° C. for 2-48 hours to obtain the lithium lanthanum zirconium oxide solid electrolyte (LLZO).

[0043] Alternatively, the preparation method of the lithium lanthanum zirconium oxide solid ...

Embodiment 1

[0049] (1) The chemical formula is Li prepared by solid-state reaction method 6.4 La 3 Zr 1.4 Ta 0.6 o 12 Lithium lanthanum zirconium oxide solid electrolyte powder, its preparation steps include: according to the molar ratio of Li, La, Zr, Ta is 6.4:3:1.4:0.6, select LiOH, La 2 o 3 , ZrO 2 and Ta 2 o 5 LiOH is used as a raw material with an excess of 5 wt% LiOH, which is ball-milled in alcohol for 24 hours and then dried; then calcined at 900 °C for 10 hours with a heating rate of 4 °C / min, and after the sintering is completed, the powder is crushed and sieved to obtain Li 6.4 La 3 Zr 1.4 Ta 0.6 o 12 Powder (LLZTO), which is sieved to obtain LLZTO powder with uniform particle size.

[0050] (2) The LLZTO powder obtained in step (1) is dispersed in a solvent, and the precursor of the cladding layer material, zirconium oxychloride ZrOCl 2 Dissolve in a solvent containing LLZTO powder, add a chelating agent to form a sol-gel, heat and evaporate the solvent to obtain...

Embodiment 2

[0057] Basically the same as embodiment 1, the difference is that the cladding layer material is the Li of NASICON structure 1.3 al 0.3 Ti 1.7 (PO 4 ) 3 (LATP). In Example 2, a surface-stabilized lithium lanthanum zirconium oxide solid electrolyte material (LATP@LLZTO) was prepared, wherein the content of the coating material LATP was 2 wt%.

[0058] Figure 6 The XRD spectrum of the prepared surface-stabilized lithium lanthanum zirconium oxide solid electrolyte material (LATP@LLZTO) was obtained by Figure 6 It can be seen that the surface-stabilized lithium lanthanum zirconium oxide solid electrolyte material (LATP@LLZTO) still maintains a cubic phase with high ionic conductivity.

[0059] Figure 7 The TEM image of the prepared surface-stabilized lithium-lanthanum-zirconium-based solid electrolyte material (LATP@LLZTO) was obtained by Figure 7 It can be seen that LATP is evenly coated on the surface of LLZTO.

[0060] Preparation of lithium-lanthanum-zirconium-bas...

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Abstract

The invention discloses a lithium-lanthanum-zirconium oxide-based solid electrolyte material with stable surface, and a preparation method and an application thereof. The solid electrolyte material comprises an inner core and a coating layer which coats the surface of the inner core; the inner core is a lithium-lanthanum-zirconium oxide-based solid electrolyte (LLZO); and a material of the coatinglayer is an oxide. The inner core part, namely, the LLZO is coated with the oxide coating layer; and the LLZO can maintain a stable three-dimensional phase structure with high ionic conductivity, sothat phase change or thermal decomposition does not occur. The material of the oxide coating layer can change the chemical composition and surface acid-base property of the surface of the LLZO, and can block the erosion of air and water to the LLZO, so that the chemical stability of the LLZO in the air and the water is greatly improved, the application range, the processing environment and the using condition of the LLZO are expanded, and the energy density and the cycling stability of a lithium-lanthanum-zirconium oxide-based battery are improved.

Description

technical field [0001] The invention relates to the technical field of batteries, in particular to a surface-stabilized lithium-lanthanum-zirconium-based solid electrolyte material and a preparation method and application thereof. Background technique [0002] The development of high-efficiency secondary battery energy storage devices is of great strategic significance for improving power balance, developing wind and solar sustainable energy, and promoting the development of new energy vehicles. Lithium-ion batteries have the advantages of high specific energy, high specific power, small self-discharge, and no memory effect, and have gradually entered the fields of electric vehicles, rail transit, and large-scale energy storage. However, safety issues have always been a major bottleneck restricting the application of lithium-ion batteries in large-scale energy storage fields such as power batteries and smart grids. Currently widely used lithium-ion batteries use volatile an...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M10/0562H01M10/0525H01M10/058H01M10/42
CPCH01M10/0562H01M10/0525H01M10/058H01M10/4235H01M2300/0077H01M2300/0094Y02P70/50
Inventor 郭向欣郭新赵宁
Owner 济宁克莱泰格新能源科技有限公司
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