Insight into the Coordination Environment of Ru Single‐Atom for Dry Reforming of Methane

Abstract Dry reforming of methane (DRM), a pivotal process for converting greenhouse gases into syngas is demanding rationally designed catalysts with high stability and ideal catalytic performance for industrial applications due to its stability of reactant molecules and characteristic of carbon deposition. However, the mechanistic understanding of how the coordination environment of the metal in a single‐atom catalytic system may influence the catalytic performance remains limited. In this work, high‐ and low‐coordinating Ru‐based (RuHC and RuLC) catalysts with distinct Ru‐O coordination numbers are prepared using one‐pot and two‐step methods. The difference in the stability (12.3% and negligible deactivation during 20 h test for RuLC and RuHC catalysts respectively) and selectivity (0.57 and 0.37 of H 2 /CO ratio) brought by the coordination environment signified the structure‐function relationship of single‐atom catalysts in DRM. The impact of the structure on the properties is systematically investigated by thorough structural and operando characterization as well as density functional theory (DFT) calculation. The findings contribute to the optimal design of single‐atom catalysts for DRM, offering a theoretical basis for industrial catalyst development and the potential to improve the process's environmental impact.