Observation of Electrochemically Driven Elemental Segregation in a Si Alloy Thin‐Film Anode and its Effects on Cyclic Stability for Li‐Ion Batteries

Abstract

The results of employing (Ti, Fe)‐alloyed Si thin‐film anode for Li‐ion batteries are reported. The material demonstrates an impressive cyclic stability with stable operation for more than 500 cycles at a capacity higher than 1400 mAh g−1. Materials characterization using scanning electron microscopy and transmission electron microscopy illuminates an intriguing materials process behind the performance: ripple‐like pattern formation via electrochemically driven segregation of the inactive elements (Ti and Fe). The ripple structure plays a buffer role by suppressing loss of the active material upon further cycling, allowing the anode to gradually transform into an array of microbumps. The morphological evolution helps the anode endure long cycles (even up to 1000 cycles) without catastrophic failure as the bumps shrank slowly and steadily, consistent with the electrochemical data.