Unraveling Anisotropic Hybridizations of Solid-state Electrolyte Nano-films in Li-ion Batteries
arxiv(2024)
Abstract
Li2WO4 (LWO) is recognized for its potential as a solid-state electrolyte and
it has demonstrated the ability to enhance the electrochemical performance of
LiCoO2 (LCO) cathodes in Li-ion batteries. However, prior investigations into
LWO have predominantly involved polycrystalline structures, thereby lacking a
comprehensive understanding of its behavior when interfaced with single crystal
systems, particularly those intricately connected to LCO. In this study, we
employ pulsed laser deposition (PLD) to epitaxially synthesize LWO nano-films
on LCO layers with different orientations. Based on a series of high-resolution
synchrotron-based techniques including X-ray absorption spectroscopy (XAS) and
X-ray photoemission spectroscopy (XPS), the electronic structure of LWO is
carefully scrutinized where a higher main energy level of W5d(eg)-O2p orbitals
hybridization in LWO/LCO(104) as compared to LWO/LCO(003) has been observed.
This experimental finding is further validated by a comprehensive set of
density of states calculations. Furthermore, detailed polarized XAS
characterization unveils distinct anisotropy between the two oriented LWO
configurations. This comprehensive scientific investigation, harnessing the
capabilities of synchrotron-based techniques, provides invaluable insights for
future studies, offering guidance for the optimized utilization of LWO as a
solid-state electrolyte or modification layer for LCO cathodes in high-powered
Li-ion batteries.
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