Lithium-lanthanum-zirconium oxide-based solid electrolyte material capable of inhibiting lithium dendrites, and preparation method and application thereof

A solid electrolyte, lithium lanthanum zirconium oxide technology, applied in the manufacture of electrolyte batteries, electrolytes, non-aqueous electrolyte batteries, etc., can solve the problems of LLZO and metal lithium wettability to be improved, battery short circuit, safety restrictions on lithium-ion batteries, etc. Achieve the effects of improving cycle stability, inhibiting growth, and preventing precipitation

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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  • 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.
However, in recent years, studies have found that when LLZO solid electrolyte ceramic sheets are assembled into metal lithium symmetric batteries Li / LLZO / Li, lithium dendrites will form inside LLZO after many cycles and cause battery short circuit; in addition, LLZO has the same wettability as metal lithium. Room for improvement

Method used

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  • Lithium-lanthanum-zirconium oxide-based solid electrolyte material capable of inhibiting lithium dendrites, and preparation method and application thereof
  • Lithium-lanthanum-zirconium oxide-based solid electrolyte material capable of inhibiting lithium dendrites, and preparation method and application thereof
  • Lithium-lanthanum-zirconium oxide-based solid electrolyte material capable of inhibiting lithium dendrites, and preparation method and application thereof

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preparation example Construction

[0040] The preparation method of the lithium-lanthanum-zirconium-based solid electrolyte material capable of suppressing lithium dendrites comprises:

[0041] (1) preparing the lithium lanthanum zirconium oxide solid electrolyte;

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

[0043] Alternatively, the preparation method of the lithium-lanthanum-zirconium-based solid electrolyte is a ...

Embodiment 1

[0049] (1) The preparation of chemical formula is Li by solid phase reaction method 6.75 La 3 Zr 1.75 Ta 0.25 o 12 Lithium-lanthanum-zirconium-based solid electrolyte powder, the preparation steps of which include: selecting LiOH, La 2 o 3 , ZrO 2 and Ta 2 o 5 LiOH is used as a raw material, in which the excess of LiOH is 5wt%, and it is ball milled in alcohol for 24 hours and then dried; then it is calcined at 900°C for 10 hours, and the heating rate is 4°C / min. After the sintering is completed, the powder is crushed and sieved to obtain Li 6.75 La 3 Zr 1.75 Ta 0.25 o 12 Powder (LLZTO).

[0050] (2) Mechanical ball milling: the coating material Li 3 PO 4 The mixed material of the precursor and the LLZTO powder obtained in step (1) is placed in a grinding tank, ethanol is added, and the mixed material is ground with grinding balls; Separator separates the ball material to obtain mixed powder; the material of the grinding ball is zirconia, the ball-to-material ra...

Embodiment 2

[0057] It is basically the same as Example 1, the difference is that the cladding layer material is Li 2 ZrO 3 , to prepare Li 2 ZrO 3 Coating modified lithium lanthanum zirconium based solid electrolyte material (Li 2 ZrO 3 @LLZTO), where the cladding material Li 2 ZrO 3 The content is 2wt%.

[0058] Figure 5 Lithium lanthanum zirconium based solid electrolyte material (Li 2 ZrO 3 XRD spectrum of @LLZTO) by Figure 5 It can be seen that the lithium-lanthanum-zirconium-based solid electrolyte material (Li 2 ZrO 3 @LLZTO) still maintains a cubic phase with high ionic conductivity.

[0059] Figure 6 Lithium lanthanum zirconium based solid electrolyte material (Li 2 ZrO 3 TEM image of @LLZTO), courtesy of Figure 6 It can be seen that Li 2 ZrO 3 The nano-thin layer is uniformly coated on the surface of LLZTO.

[0060] Preparation of lithium lanthanum zirconium oxide ceramic sheets by hot pressing sintering method: Li 2 ZrO 3 @LLZTO powder is put into the mo...

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Abstract

The invention discloses a lithium-lanthanum-zirconium oxide-based solid electrolyte material capable of inhibiting lithium dendrites, and a preparation method and an application thereof. The lithium-lanthanum-zirconium oxide-based solid electrolyte material capable of inhibiting the lithium dendrites comprises an inner core and a coating layer which coats the surface of the inner core; the core isa lithium-lanthanum-zirconium oxide-based solid electrolyte (LLZO); and a material of the coating layer is a lithium-containing oxide and/or a non-oxidized lithium-containing compound. The surface ofthe lithium-lanthanum-zirconium oxide-based solid electrolyte is coated with the lithium-containing compound, so that a contact layer between the LLZO and a metal lithium interface is a pure ion conductor, electrons can be prevented from being transmitted to the surface of the LLZO, metal lithium is prevented from being separated out on the surface of the LLZO, and the growth of the dendrites towards the inside of a volume phase of the LLZO is inhibited. In addition, the coating layer can react with the metal lithium to generate an interface fusion intermediate layer for enhancing the ion transport capacity; and the interface fusion intermediate layer is an ideal interface of the metal lithium and the LLZO, so that the cycling stability of the battery can be improved.

Description

technical field [0001] The invention relates to the technical field of batteries, in particular to a lithium-lanthanum-zirconium-based solid electrolyte material capable of suppressing lithium dendrites 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 bat...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M10/0562H01M10/0525H01M10/058H01M10/42
CPCH01M10/0562H01M10/0525H01M10/058H01M10/4235H01M2300/0077H01M2300/0094Y02E60/10Y02P70/50
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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