Revolutionary Insights into the Material Structure Design Enabled by Single-Atom Catalysts

Single-atom catalysts (SACs) propel catalytic science into the era of atomic manufacturing. Today, synthesizing SACs extends beyond anchoring atomically dispersed metal atoms, increasingly focusing on the synergistic integration of single-atom active sites with other functional components. More significantly, single-atom active sites provide an ideal platform for validating catalytic reaction mechanisms, having triggered intense discussions and revolutionary insights in recent years. Consequently, this review comprehensively examines both classical and recently developed SAC architectures, while systematically summarizing reaction mechanisms based on these structures, including coordination engineering, dynamic coordination, metal–support interaction, d–p orbital hybridization, spin active centers, asymmetric active centers, f-block elements, pathway synergy, and distance effect. These mechanistic principles establish targeted design objectives for atomic structures of efficient catalysts and furnish atomic-level blueprints for materials genome initiatives.