Hydroxyl Group-Regulated Active Nano-Pd/C Catalyst Generation via in Situ Reduction of Pd(NH3)xCly/C for N-Formylation of Amines with CO2/H2

The reductive N-formylation of amines using CO2 and hydrogen is a promising means of incorporating CO2 into value-added chemicals. To date, there has been a lack of heterogeneous catalyst systems that are sufficiently active and selective for N-formylation of primary amines with CO2 and H2. For the first time, we report that a highly active palladium nanoparticle supported on an hydroxyl group-functionalized carbon material has been designed for the N-formylation of aliphatic primary amines with CO2 and H2. XPS, XRD, FT-Raman, and TEM characterizations revealed the adsorbing of Pd(NH3)xCly onto the carbon support during catalyst preparation, followed by in situ reduction to generate active nano-Pd particles. The catalytic activity of the Pd/C catalysts can be tuned efficiently by the hydroxyl group, which can modulate the hydrophilic/hydrophobic properties of the carbon surface, and promote the adsorption of CO2 and the amines near the Pd sites. The results described here may promote the design of an active catalyst for CO2 recycling and N-formyl amine synthesis.