A long-range synergistic effect between Ptn clusters and Zn1 single atoms for efficient selective hydrogenations†

Abstract

Supported platinum group metal (PGM) catalysts are extensively utilized in catalytic hydrogenations. However, the adsorption energies on single PGM surfaces present the inherent scaling properties, which often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy by confining few-atom Pt_n clusters in Zn₁-N₃ sites decorated with microporous carbon material (Pt_n@Zn₁-N–C) to break the scaling relationship in selective hydrogenations. In detail, Pt_n clusters are more favorable for H₂ activation, while the Zn₁-N₃ single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atoms. Benefiting from this long-range synergistic effect, the Pt_n@Zn₁-N–C catalyst displays superior catalytic performance in the selective hydrogenation of nitroarenes (>99% selectivity at ∼100% conversion, and sulfur compound-resistant hydrogenations) and excellent stability in the reverse water gas shift reaction (>99% selectivity over 40 hours at 600 °C). Our findings provide a confinement approach for further improving catalytic performance in selective hydrogenations.