Tandem Nitrogen Functionalization of Porous Carbon: Toward Immobilizing Highly Active Palladium Nanoclusters for Dehydrogenation of Formic Acid

Highly dispersed palladium nanoclusters (Pd NCs) immobilized by a nitrogen (N)-functionalized porous carbon support (N-MSC-30) are synthesized by a wet chemical reduction method, wherein the N-MSC-30 prepared by a tandem low-temperature heat-treatment approach proved to be a distinct support for stabilizing the Pd NCs. The prepared Pd/N-MSC-30 shows extremely high catalytic activity and recyclability for the dehydrogenation of formic acid (FA), affording the highest turnover frequency (TOF = 8414 h–1) at 333 K, which is much higher than that of the Pd catalyst supported on the N-MSC-30 prepared via a one-step process. This tandem heat-treatment strategy provides a facile and effective synthetic methodology to immobilize ultrafine metal NPs on N-functionalized carbon materials, which have tremendous application prospects in various catalytic fields.