Enhanced Catalytic Performance of N‑Doped Carbon Sphere-Supported Pd Nanoparticles by Secondary Nitrogen Source Regulation for Formic Acid Dehydrogenation

The development of catalysts with high selectivity, good catalytic activity, and excellent cycle performance is of significance for the application of formic acid (HCOOH, FA) as a hydrogen support. Herein, Pd is deposited on a series of N-doped carbons, which are prepared by cocarbonization of N-containing zeolite imidazole frameworks (ZIF-8) and other N/C sources (melamine, xylitol, urea, and glucose), for hydrogen generation from FA. The results demonstrate that the introduction of a secondary N/C source further affects the catalytic performance of Pd by adjusting the morphology, specific surface area, N content, and type of carbon. The effects of N atoms and the favorable reaction pathways of FA dehydrogenation were revealed by theoretical calculation. This work will improve the understanding of N doping on the decomposition mechanism of FA and provide a new approach for the rational design of metal-N-C materials.