First-principles calculation on the lithium storage properties of high-entropy MXene Ti3C2(N0.25O0.25F0.25S0.25)2

Experimental studies had shown that a variety of surface functional groups exist simultaneously on the surface of Ti3C2Tx MXenes. However, current theoretical calculations on MXenes, used as anode materials for lithium-ion batteries, consider only one surface functional group, which fails to take into account the actual situation. In this study, combining the characteristics of high-entropy materials and two-dimensional MXene material, a model of MXene with multiple surface functional groups was constructed, and its electrochemical performance as an anode material for lithium-ion batteries was further explored. The Ti3C2(N0.25O0.25F0.25S0.25)2 monolayer exhibited metallic properties. Meanwhile, Li atoms could be stably adsorbed on the surface and the diffusion energy barrier of Li on the surface was only 0.17 eV. First-principles calculation showed that Ti3C2(N0.25O0.25F0.25S0.25)2 monolayer had good rate performance and low open-circuit voltage (1 V), corresponding to a lithium storage capacity of 385.38 mA h g-1. The results of our work might inspire further studies on the Li storage performance of high-entropy MXenes experimentally and theoretically.