Designing a Robust Palladium Catalyst for Formic Acid Dehydrogenation

The efficient production of hydrogen from biomass- or CO2-derived formic acid (FA) is of considerable attention for a competitive hydrogen-powered economy. In this study, we report the synthesis of effective palladium catalysts with tunable metal-support interaction and electronic properties via a stepwise annealing and reduction strategy. Highly dispersed Pd nanoparticles on carbon nitride with a moderate average charge were identified as the optimal system. This material exhibits an increased rate of gas formation under standard conditions by two orders of magnitude compared to the commercially available benchmark catalyst (Pd/C). The activity was further improved by optimally adjusting the effects of solvent, temperature, amount of FA, and additive, reaching a maximum of 1.46 L gcat–1 h–1. The state-of-the-art catalyst shows superior long-term stability and is still active after 15 days of operation, achieving the highest total turnover number of 41,395 of any known palladium system.