posted on 2023-01-03, 16:06authored byAshley Cronk, Yu-Ting Chen, Grayson Deysher, So-Yeon Ham, Hedi Yang, Phillip Ridley, Baharak Sayahpour, Long Hoang Bao Nguyen, Jin An Sam Oh, Jihyun Jang, Darren H. S. Tan, Ying Shirley Meng
All-solid-state batteries (ASSBs) are one of the most
promising
systems to enable long-lasting and thermally resilient next-generation
energy storage. Ideally, these systems should utilize low-cost resources
with reduced reliance on critical materials. Pursuing cobalt- and
nickel-free chemistries, like LiFePO4 (LFP), is a promising
strategy. Morphological features of LFP essential for improved electrochemical
performance are highlighted to elucidate the interfacial challenges
when implemented in ASSBs, since adoption in inorganic ASSBs has yet
to be reported. In this work, the compatibility of LFP with two types
of solid-state electrolytes, Li6PS5Cl (LPSCl)
and Li2ZrCl6 (LZC), are investigated. The potential
existence of oxidative decomposition products is probed using a combination
of structural, electrochemical, and spectroscopic analyses. Bulk and
interfacial characterization reveal that the sulfide-based electrolyte
LPSCl decomposes into insulative products, and electrochemical impedance
spectroscopy is used to quantify the resulting impedance growth. However,
through utilization of the chloride-based electrolyte LZC, high-rate
and stable electrochemical performance is achieved at room temperature.