Pd single-atom monolithic catalyst: Functional 3D structure and unique chemical selectivity in hydrogenation reaction

Abstract

Regulating the selectivity of catalysts in selective hydrogenation reactions at the atomic level is highly desirable but remains a grand challenge. Here we report a simple and practical strategy to synthesize a monolithic single-atom catalyst (SAC) with isolated Pd atoms supported on bulk nitrogen-doped carbon foams (Pd-SAs/CNF). Moreover, we demonstrate that the single-atom Pd sites with unique electronic structure endow Pd-SAs/CNF with an isolated site effect, leading to excellent activity and selectivity in 4-nitrophenylacetylene semi-hydrogenation reaction. In addition, benefiting from the great integrity and excellent mechanical strength, monolithic Pd-SAs/CNF catalyst is easy to separate from the reaction system for conducting the subsequent recycling. The cyclic test demonstrates the excellent reusability and stability of monolithic Pd-SAs/CNF catalyst. The discovery of isolated site effect provides a new approach to design highly selective catalysts. And the development of monolithic SACs provides new opportunities to advance the practical applications of single-atom catalysts.