Long-Range Synergistic Effect between Ptn Cluster and Zn1 Single Atom for Efficient Selective Hydrogenations

Abstract

Supported platinum group metals (PGMs) catalysts are extensively utilized in catalytic hydrogenations. However, the inherent scaling properties of adsorption energies on single PGM surfaces often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy, via confining few-atom Ptn clusters in Zn1-N3 sites decorated micropore carbon material (Ptn@Zn1-N-C), to break the scaling relationship in selective hydrogenations. In detail, the Ptn clusters are more favorable for H2 activation, and the Zn1-N3 single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atom. Benefit from this long-range synergistic effect, Ptn@Zn1-N-C catalyst displays the superior catalytic performance in selective hydrogenation of nitroarenes (>99% selectivity at ~100% conversion, and sulfur compound-resistant hydrogenations) and the excellent stability in 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.