Among the main appeals of single-atom catalysts are the ultimate efficiency of material utilization and the well-defined nature of the active sites, holding the promise of rational catalyst design. A major challenge is the stable decoration of various substrates with a high density of individually dispersed and uniformly active monatomic sites. Transition metal chalcogenides (TMCs) are broadly investigated catalysts, limited by the relative inertness of their pristine basal plane. We propose that TMC single layers modified by substitutional heteroatoms can harvest the synergistic benefits of stably anchored single-atom catalysts and activated TMC basal planes. These solid-solution TMC catalysts offer advantages such as simple and versatile synthesis, unmatched active site density, and a stable and well-defined single-atom active site chemical environment. The unique features of heteroatom-doped two-dimensional TMC crystals at the origin of their catalytic activity are discussed through the examples of various TMC single layers doped with individual oxygen heteroatoms.
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