LAUSR

Abstract Chemical bonding has been regarded as an effective modification strategy to enhance the electrochemical performance of MXenes for Li-ion batteries (LIBs). However, the in-depth mechanism, especially concentrating on the regulation of chemical bond, is rarely explored. Herein, we design an atomically dispersed Fe in Ti3C2Tx MXene (Fe-Ti3C2Tx) by a doping route and the underlying mechanism of high-capacity LIBs is comprehensively investigated. Density functional theory (DFT) calculations reveal that unsaturated O coordination can be induced by electron transfer on Fe−O bond, which enables improved Li-ion adsorption on the surface of Fe-Ti3C2Tx nanosheet during charge/discharge process. The experimental observations from X-ray photoelectron spectroscopy (XPS) confirm the successful introduction of Fe atoms into intrinsic structure of Ti3C2Tx MXene, and the X-ray absorption spectroscopy (XAS) data verify the electron tranfer of Fe−O bond. Moreover, Fe-Ti3C2Tx electrode exhibits greatly enhanced electrochemical performance (564.9 mAh g-1 at 50 mA g-1 under -10 °C), surpassing that of pristine Ti3C2Tx (77 mAh g-1). The cycling stability of Fe-Ti3C2Tx over 500 cycles (418.8 mAh g-1 at 200 mA g-1 under -10 °C). This work is expected to provide a guideline to develop brand-new MXene-based electrode materials with high-capacity for energy storage.