Electrospinning Synthesis of N-Doped Graphene Encapsulated Feconicrcu High-Entropy Alloy Nanoparticles for Efficient Nitrobenzene Hydrogenation

Abstract

Selective reduction of aromatic nitro compounds to functionalized anilines remains a formidable challenge due to the competitive reducible functional groups. High-entropy alloys (HEAs) with multiple elements in near-equiatomic proportions hold great promise given their exceptional physicochemical properties. Herein, we developed nitrogen-doped carbon nanofiber-encapsulated HEA nanoparticles (FeCoNiCrCu@N-CNFs) for efficient nitrobenzene hydrogenation to aniline. The FeCoNiCrCu@N-CNFs catalyst demonstrated exceptional activity with 99% aniline yield at 60℃, outperforming the FeCoNi@N-CNFs counterpart by a factor of 6.6. The HEA-NC heterojunction was constructed on the surface of the catalyst given the intimate contact between the N-doped carbon layer and the alloy particles. Density functional theory (DFT) calculations revealed that the elevated d-band center of the HEA, induced by carbon interaction, enhances the intermediates adsorption. This synergistic interplay between HEA and nitrogen-doped carbon provides a novel strategy for designing selective hydrogenation catalysts.

Keywords: High-entropy alloys, N-doped carbon, Hydrogenation of nitroaromatic hydrocarbons, Electrospun