Spillover Dynamics in Heterogeneous Catalysis on Singe‐Atom Alloys: A Theoretical Perspective

ABSTRACT Recent advances in single‐atom alloy ( SAA ) catalysts provide a unique platform for understanding spillover, due to the well‐defined nature of the active site for dissociative chemisorption. In particular, the use of spilled adsorbates following molecular dissociation on the host metal surface facilitates the generation of high‐value chemicals in subsequent catalytic reactions. Nevertheless, the factors that control the spillover process remain to be fully elucidated. This perspective discusses recent theoretical advances in the spillover dynamics on SAAs , with a particular focus on the dissociation and spillover processes of H 2 and CH 4 . It provides valuable insights into how various factors, such as energy transfer, nuclear quantum effects, gas‐adsorbate interactions, and adsorbate size, impact the diffusion behavior of hydrogen and methyl species on SAA surfaces. The article concludes with a discussion of future prospects. This perspective underscores the significance of spillover dynamics in heterogeneous catalysis, with important implications for improving catalytic performance.