Atomic Insights into Synergistic Nitroarene Hydrogenation over Nanodiamond-Supported Pt-1-Fe-1 Dual-Single-Atom Catalyst

Fundamental understanding of the synergistic effect of bimetallic catalysts is of extreme significance in heterogeneous catalysis, but a great challenge lies in the precise construction of uniform dual-metal sites. Here, we develop a novel method for constructing Pt-1-Fe-1/ND dual-single-atom catalyst, by anchoring Pt single atoms on Fe-1-N-4 sites decorating a nanodiamond (ND) surface. Using this catalyst, the synergy of nitroarenes selective hydrogenation is revealed. In detail, hydrogen is activated on the Pt-1-Fe-1 dual site and the nitro group is strongly adsorbed on the Fe-1 site via a vertical configuration for subsequent hydrogenation. Such synergistic effect decreases the activation energy and results in an unprecedented catalytic performance (3.1 s(-1) turnover frequency, ca. 100 % selectivity, 24 types of substrates). Our findings advance the applications of dual-single-atom catalysts in selective hydrogenations and open up a new way to explore the nature of synergistic catalysis at the atomic level.

Automated summary

Understanding the synergistic effect of bimetallic catalysts is crucial in heterogeneous catalysis. However, constructing uniform dual-metal sites is a significant challenge. In this study, a new method for constructing Pt-1-Fe-1/ND dual-single-atom catalyst was developed using nanodiamond (ND) surface decorated with Fe-1-N-4 sites. The catalyst exhibited excellent catalytic performance in nitroarenes selective hydrogenation. The findings advance the application of dual-single-atom catalysts and provide insights into synergistic catalysis at the atomic level.