Efficient Reversible Conversion between MoS₂ and Mo/Na₂S Enabled by Graphene-Supported Single Atom Catalysts

Sodium-ion batteries (SIBs) based on conversion-type metal sulfide (MS) anodes have attracted extraordinary attention due to relatively high capacity and intrinsic safety. The highly reversible conversion of M/Na₂S to pristine MS in charge plays a vital role with regard to the electrochemical performance. Here, taking conventional MoS₂ as an example, guided by theoretical simulations, a catalyst of iron single atoms on nitrogen-doped graphene (SAFe@NG) is selected and first used as a substrate to facilitate the reaction kinetics of MoS₂ in the discharging process. In the following charging process, using a combination of spectroscopy and microscopy, it is demonstrated that the SAFe@NG catalyst enables an efficient reversible conversion reaction of Mo/Na₂S→NaMoS₂→MoS₂. Moreover, theoretical simulations reveal that the reversible conversion mechanism shows favorable formation energy barrier and reaction kinetics, in which SAFe@NG with the Fe–N₄ coordination center facilitates the uniform dispersion of Na₂S/Mo and the decomposition of Na₂S and NaMoS₂. Therefore, efficient reversible conversion reaction MoS₂↔NaMoS₂↔Mo/Na₂S is enabled by the SAFe@NG catalyst. This work contributes new avenues for designing conversion-type materials with an efficient reversible mechanism.