4.8 Article

Building an Air Stable and Lithium Deposition Regulable Garnet Interface from Moderate-Temperature Conversion Chemistry

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 29, Pages 12069-12075

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202003177

Keywords

contaminations; electrochemical energy storage; fluorinated interface; garnet electrolyte; solid-state batteries

Funding

  1. Basic Science Center Project of National Natural Science Foundation of China [51788104]
  2. National Key R&D Program of China [2016YFA0202500]
  3. National Natural Science Foundation of China [21975266, 21773264]
  4. Beijing Natural Science Foundation [L172023]
  5. Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences [XDA 21070300]
  6. Recruitment Program of Global Youth Experts of China
  7. Chinese Academy of Sciences

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Garnet-type electrolytes suffer from unstable chemistry against air exposure, which generates contaminants on electrolyte surface and accounts for poor interfacial contact with the Li metal. Thermal treatment of the garnet at >700 degrees C could remove the surface contaminants, yet it regenerates the contaminants in the air, and aggravates the Li dendrite issue as more electron-conducting defective sites are exposed. In a departure from the removal approach, here we report a new surface chemistry that converts the contaminants into a fluorinated interface at moderate temperature <180 degrees C. The modified interface shows a high electron tunneling barrier and a low energy barrier for Li+ surface diffusion, so that it enables dendrite-proof Li plating/stripping at a high critical current density of 1.4 mA cm(-2). Moreover, the modified interface exhibits high chemical and electrochemical stability against air exposure, which prevents regeneration of contaminants and keeps high critical current density of 1.1 mA cm(-2). The new chemistry presents a practical solution for realization of high-energy solid-state Li metal batteries.

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