On-surface lithium donor reaction enables decarbonated lithium garnets and compatible interfaces within cathodes.

Yang, Ya-Nan; Li, Ying-Xiang; Li, Yi-Qiu; Zhang, Tao · Nat Commun · 2020

basic_science · Level V

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Abstract

Lithium garnets have been widely studied as promising electrolytes that could enable the next-generation all-solid-state lithium batteries. However, upon exposure to atmospheric moisture and carbon dioxide, insulating lithium carbonate forms on the surface and deteriorates the interfaces within electrodes. Here, we report a scalable solid sintering method, defined by lithium donor reaction that allows for complete decarbonation of Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) and yields an active LiCoO<sub>2</sub> layer for each garnet particle. The obtained LiCoO<sub>2</sub> coated garnets composite is stable against air without any Li<sub>2</sub>CO<sub>3</sub>. Once working in a solid-state lithium battery, the LiCoO<sub>2</sub>-LLZTO@LiCoO<sub>2</sub> composite cathode maintains 81% of the initial capacity after 180 cycles at 0.1 C. Eliminating CO<sub>2</sub> evolution above 4.0 V is confirmed experimentally after transforming Li<sub>2</sub>CO<sub>3</sub> into LiCoO<sub>2</sub>. These results indicate that Li<sub>2</sub>CO<sub>3</sub> is no longer an obstacle, but a trigger of the intimate solid-solid interface. This strategy has been extended to develop a series of LLZTO@active layer materials.