Abstract

<h2>Summary</h2> The realization of lithium-ion battery (LIB) anodes with high volumetric energy densities and minimal Li plating at high rates remains a key challenge for emerging technologies, including electric vehicles and grid-level energy storage. Here, we present graphene-functionalized Li<sub>2</sub>TiSiO<sub>5</sub> (G-LTSO) as a high volumetric energy and power density anode for LIBs. G-LTSO forms a dense electrode structure with electronically and ionically conductive networks that deliver superior electrochemical performance. Upon lithiation, <i>in situ</i> transmission electron microscopy reveals that graphene functionalization yields minimal structural changes compared with pristine LTSO, resulting in high cycling stability. Furthermore, G-LTSO exhibits not only high charge and discharge capacities but also low overpotentials at high rates with minimal voltage fading due to reduced formation of a solid-electrolyte interphase. The combination of highly compacted electrode morphology, stable high-rate electrochemistry, and low operating potential enables G-LTSO to achieve exceptional volumetric energy and power densities that overcome incumbent challenges for LIBs.

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