Lithium storage properties of Ti3C2T (T = F, Cl, Br) MXenes

In this work, Ti3C2Tx MXene with -F, -Cl and -Br surface terminations are synthesized and the effect of these halogen terminations on the lithium storage properties is investigated. A maximum Li+ storage capacity of 189 mAh/g is achieved with Ti3C2Brx MXene much higher than Ti3C2Clx and Ti3C2Fx with 138 mAh/g and 123 mAh/g, respectively. Density functional theory (DFT) calculation shows that the adsorption formation energy of halogen atoms on Ti atoms follows the trend of Ti-F > Ti-Cl > Ti-Br, leading to the same trend in the content of terminations on corresponding MXenes. In addition, inevitable exposure of MXene to oxygen causes competition between halogen and oxygen. Theoretical results show Ti3C2Brx MXene has the highest Ti to O ratio and the lowest Ti to Br ratio, the high lithium affinity of O explains the maximum Li-ion storage capacity with Ti3C2Brx MXene. This work shed light on the opportunity for achieving improved lithium storage properties of MXene electrodes by regulating the surface chemistry.