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Abstract
Garnet based solid-state batteries have the advantages of wide electrochemical window and good chemical stability. However, at Li-garnet interface, the poor interfacial wettability due to Li2CO3 passivation usually causes large resistance and unstable contact. Here, a Li2CO3-affiliative mechanism is proposed for air-accessible interface engineering of garnet electrolyte via facile liquid metal (LM) painting. The natural LM oxide skin enables a superior wettability of LM interlayer towards ceramic electrolyte and Li anode. Therein the removal of Li2CO3 passivation network is not necessary, in view of its delamination and fragmentation by LM penetration. This dissipation effect allows the lithiated LM nanodomains to serve as alternative Li-ion flux carriers at Li-garnet interface. This mechanism leads to an interfacial resistance as small as 5 Ω cm2 even after exposing garnet in air for several days. The ultrastable Li plating and stripping across LM painted garnet can last for 9930 h with a small overpotential.
At Li-garnet interface, the poor interfacial wettability due to Li2CO3 passivation causes large resistance and unstable contact. Here the authors propose a Li2CO3-affiliative mechanism for air-accessible interface engineering of garnet electrolyte with superior wettability via facile liquid metal painting.
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1 Shanghai Institute of Ceramics, Chinese Academy of Sciences, State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai, China (GRID:grid.454856.e) (ISNI:0000 0001 1957 6294); University of Chinese Academy of Sciences, Center of Materials Science and Optoelectronics Engineering, Beijing, China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419)
2 Shanghai Institute of Ceramics, Chinese Academy of Sciences, State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai, China (GRID:grid.454856.e) (ISNI:0000 0001 1957 6294)