Tailoring the Electronic Metal‐Support Interaction of Single‐Atom Platinum Catalysts for Boosting Water‐Gas Shift Reaction

Abstract Exploring electronic metal‐support interaction (EMSI) in heterogeneous catalysis is significant for developing efficient supported metal catalysts. Herein, single‐atom Pt 1 /CeO 2 catalysts possessing diverse local structures and coordination environments are convincingly fabricated via ALD technique for the water‐gas shift reaction (WGSR). The PtCe‐2 catalyst obtained after two ALD cycles is primarily composed of Pt 1 coordinated to five oxygen atoms (Pt 5c ), while the PtCe‐6 catalyst is dominated by Pt 3c configuration. The PtCe‐2 catalyst exhibits an H 2 production rate ≈2.4 times higher than that of PtCe‐6 at 250 °C. The combined experimental and theoretical studies demonstrate that the atomic location‐induced strong EMSI weakens the adsorption strength of CO on Pt 5c , subsequently lowering the energy barrier for the crucial intermediate step of CO conversion. This study elucidates the effect of EMSI in the WGSR, and provides new insights for the rational design of efficient single‐atom catalysts.