Constructing a Micrometer-Sized Structure through an Initial Electrochemical Process for Ultrahigh-Performance Li⁺...

Orthorhombic niobium pentoxide (T-Nb₂O₅) is a promising anode to fulfill the requirements for high-rate Li-ion batteries (LIBs). However, its low electric conductivity and indistinct electrochemical mechanism hinder further applications. Herein, we develop a novel method to obtain a micrometer-sized layer structure of S-doped Nb₂O₅ on an S-doped graphene (SG) surface (the composite is denoted S-Nb₂O₅/SG) after the initial cycle, which we call "in situ electrochemically induced aggregation". In situ and ex situ characterizations and theoretical calculations were carried out to reveal the aggregation process and Li⁺ storage process. The unique merits of the composite with a micrometer-sized layer structure increased the reaction degree, structural stability, and electrochemical kinetics. As a result, the electrode exhibited a large capacity (∼598 mAh g^-1 at 0.1 A g^-1), outstanding cycling stability (∼313 mAh g^-1 at 5 A g^-1 and remains at ∼313 mAh g^-1 after 1000 cycles), and a high Coulombic efficiency and has a high fast-charging performance and excellent cycling stability.