Atomic‐Level Engineering of Transition Metal Dichalcogenides for Enhanced Hydrogen Evolution Reaction

Abstract 2D transition metal dichalcogenides (2D‐TMDs) have attracted considerable attention due to their characteristic layered structures, which provide abundant accessible surface sites. Significant research efforts are dedicated to designing nanostructures and regulating electron properties to enhance the catalytic performance of the hydrogen evolution reaction (HER) of TMDs. However, elucidating the HER mechanism, particularly the role of active sites, remains challenging owing to the complex surface and electronic structures introduced by nanoscale modification. Recent advances have focused on achieving efficient HER catalysis through atomic‐level control of TMD surface structures and precise identification of the coordination environment of active sites. Atomic‐level engineering of TMDs, including incorporating or removing specific atoms onto the basal surfaces or within the interlayer via advanced synthetic approaches, has emerged as a promising strategy. These modifications optimize the adsorption/desorption energy of H, increase the density of active sites, and create synergetic active sites by arranging atoms in controlled configuration, in single‐atomic modified TMDs (SA‐TMDs) catalysts. Further, the insights of a notable increase of HER performance in SA‐TMDs are discussed in detail when compared to both their pure and conventionally doped counterparts. This review aims to advance the understanding of atomic‐level catalysis and provides a basis for developing next‐generation materials for energy applications.