Journal
ADVANCED MATERIALS
Volume 32, Issue 23, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202000030
Keywords
garnet electrolytes; interfacial chemistry; lithium dendrites; solid-electrolyte interphase; solid-state batteries
Categories
Funding
- Office of Vehicle Technologies of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program [DE-AC02-05CH11231]
- Engie Chuck Edwards Memorial Fellowship at the University of Maryland
- Maryland NanoCenter and its AIM Lab
- Vehicle Technology Office of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program, Battery500 Consortium [DE-SC0012704]
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Lithium (Li) metal is a promising candidate as the anode for high-energy-density solid-state batteries. However, interface issues, including large interfacial resistance and the generation of Li dendrites, have always frustrated the attempt to commercialize solid-state Li metal batteries (SSLBs). Here, it is reported that infusing garnet-type solid electrolytes (GSEs) with the air-stable electrolyte Li3PO4 (LPO) dramatically reduces the interfacial resistance to approximate to 1 omega cm(2) and achieves a high critical current density of 2.2 mA cm(-2) under ambient conditions due to the enhanced interfacial stability to the Li metal anode. The coated and infused LPO electrolytes not only improve the mechanical strength and Li-ion conductivity of the grain boundaries, but also form a stable Li-ion conductive but electron-insulating LPO-derived solid-electrolyte interphase between the Li metal and the GSE. Consequently, the growth of Li dendrites is eliminated and the direct reduction of the GSE by Li metal over a long cycle life is prevented. This interface engineering approach together with grain-boundary modification on GSEs represents a promising strategy to revolutionize the anode-electrolyte interface chemistry for SSLBs and provides a new design strategy for other types of solid-state batteries.
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