V-Promoted Ultrasmall Pd Nanoparticles Supported on V-KIT-6 for the Enhanced Catalytic Dehydrogenation of Perhydro-N-ethylcarbazole

The facile catalytic dehydrogenation of LOHCs using a highly active, selective, and stable catalyst holds excellent potential for large-scale hydrogen energy applications. Here, we design and synthesize a V-decorated Pd/V-KIT-6 with ultrasmall (2.0 nm) and stable Pd nanoparticles, which enables a fast dehydrogenation of perhydro-N-ethylcarbazole (12H-NEC) with 5.8 wt % H2 release. Notably, the Pd/V-KIT-6 catalyst exhibits superior catalytic performance compared to the pure Pd/KIT-6 catalyst and some state-of-the-art noble metal catalysts. The outstanding catalytic efficiency of the Pd/V-KIT-6 catalyst is due to the optimal electronic structure and appropriate Pd0/Pdδ+ ratio induced by the VOx species, which enables rapid interfacial electron transfer, leading to the improved adsorption/desorption energy, reaction energy, kinetics data, and antitoxicity ability. The probable mechanism of V-promoted Pd catalyzed 12H-NEC dehydrogenation was thoroughly investigated and discussed by experimental analysis and density functional theory (DFT) simulations.