Carbon-Doped TiNb2O7 Suppresses Amorphization-Induced Capacity Fading.

ABSTRACT

The limited capacity of graphite anodes in high-performance batteries has led to considerable interest in alternative materials in recent years. Due to its high capacity, titanium niobium oxide (TiNb2O7, TNO) with a Wadsley-Roth crystallographic sheared structure holds great promise as a next-generation anode material, but a comprehensive understanding of TNO's electrochemical behavior is lacking. In particular, the mechanism responsible for the capacity fading of TNO remains poorly elucidated. Given its metastable nature (as an entropy-stabilized oxide) and the large volume change in TNO upon lithiation and delithiation, which has long been overlooked, the factors governing capacity fading warrant investigation. Our studies reveal that the structural weakness of TNO is fatal to the long-term cycling stability of TNO and that the capacity fading of TNO is driven by amorphization, which results in a significant increase in impedance. While nanostructuring can kinetically boost lithium intercalation, this benefit comes at the expense of capacity fading. Carbon doping in TNO can effectively suppress the critical impedance increase despite the amorphization, providing a possible remedy to the stability issue.