Understanding the dehydrogenation mechanism over iron nanoparticles catalysts based on density functional theory

The conversion of chemical feedstock materials into high value-added products accompanied with dehydrogenation is of great value in the chemical industry. However, the catalytic dehydrogenation reaction is inhibited by a limited number of expensive noble metal catalysts and lacks understanding of dehydrogenation mechanism. Here, we report the use of heterogeneous non-noble metal iron nanoparticles (NPs) incorporated mesoporous nitrogen-doped carbon to investigate the dehydrogenation mechanism based on experiment observation and density functional theory (DFT) method. Fe NPs catalyst displays excellent performance in the dehydrogenation of 1,2,3,4-tetrahydroquinoline (THQ) with 100% selectivity and 100% conversion for 10-12 h at room temperature. The calculated adsorption energy implies that THQ prefers to adsorb on Fe NPs as compared with absence of Fe NPs. What is more, the energy barrier of transition state is relatively low, illustrating the dehydrogenation is feasible. This work provides an atomic scale mechanism guidance for the catalytic dehydrogenation reaction and points out the direction for the design of new catalysts.