In
this study, we synthesize two layered and amorphous structures
of germanium phosphide (GeP5) and compare their electrochemical
performances to better understand the role of layered, crystalline
structures and their ability to control large volume expansions. We
compare the results obtained with those of previous, conventional
viewpoints addressing the effectiveness of amorphous phases in traditional
anodes (Si, Ge, and Sn) to hinder electrode pulverization. By means
of both comprehensive experimental characterizations and density functional
theory calculations, we demonstrate that layered, crystalline GeP5 in a hybrid structure with multiwalled carbon nanotubes exhibits
exceptionally good transport of electrons and electrolyte ions and
tolerance to extensive volume changes and provides abundant reaction
sites relative to an amorphous structure, resulting in a superior
solid-electrolyte interphase layer and unprecedented initial Coulombic
efficiencies in both Li-ion and Na-ion batteries. Moreover, the hybrid
delivers excellent rate-capability (symmetric and asymmetric) performance
and remarkable reversible discharge capacities, even at high current
rates, realizing ultradurable cycles in both applications. The findings
of this investigation are expected to offer insights into the design
and application of layered materials in various devices.
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