Regulating Inorganic and Organic Components to Build Amorphous-ZnF x Enriched Solid-electrolyte Interphase for Highly Reversible Zn Metal Chemistry.
Guojin LiangZijie TangBing HanJiaxiong ZhuAo ChenQing LiZe ChenZhaodong HuangXinliang LiQi YangChunyi ZhiPublished in: Advanced materials (Deerfield Beach, Fla.) (2023)
The introduction of inorganic crystallites into a solid-electrolyte interphase (SEI) is an effective strategy for improving the reversibility of Zn metal anode (ZMA). However, the structure-performance relationship of the SEI is not fully understood because the existing forms of its inorganic and organic components in their pristine states have not been resolved. Here, we constructed a highly effective SEI for ZMA using a bisolvent electrolyte and resolved its composition/structure by cryogenic transmission electron microscopy. This highly fluorinated SEI with amorphous inorganic ZnF x uniformly distributed in the organic matrix was largely different from the common mosaic and multilayer SEIs with crystalline inorganics. It featured improved structural integrity, mechanical toughness, and Zn 2+ ion conductivity. Consequently, the ZMA exhibited excellent reversibility with an enhanced plating/stripping Coulombic efficiency of 99.8%. The ZMA-based full cell achieved a high Zn utilization ratio of 54% at a practical areal capacity of 3.2 mAh cm -2 and stable cycling over 1800 h during which the accumulated capacity reached 5600 mAh cm -2 . This research highlights the detailed structure and composition of amorphous SEIs for highly reversible metal anodes. This article is protected by copyright. All rights reserved.