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

Exploring electronic metal-support interaction (EMSI) in heterogeneous catalysis is significant for developing efficient supported metal catalysts. Herein, single-atom Pt1/CeO2 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 Pt1 coordinated to five oxygen atoms (Pt5c), while the PtCe-6 catalyst is dominated by Pt3c configuration. The PtCe-2 catalyst exhibits an H2 production rate approximate to 2.4 times higher than that of PtCe-6 at 250 degrees C. The combined experimental and theoretical studies demonstrate that the atomic location-induced strong EMSI weakens the adsorption strength of CO on Pt5c, 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. The electronic metal-support interaction modulation of single-atom platinum catalysts is achieved by the atomic layer deposition technique. Notably, the H2 production rate of the PtCe-2 catalyst primarily composed of 5-coordinated single-atom Pt (Pt5c) is 2.4 times higher than that of the PtCe-6 catalyst dominated by Pt3c configuration in low-temperature water-gas shift reaction at 250 degrees C. image