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

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Abstract

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.

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