Enhanced Activity in Benzyl Alcohol Oxidation via Nitrogen-Doped Carbon-Supported Ultrahigh Dispersion of Iron Atom Catalysts

Abstract

The selective oxidation of benzyl alcohol to benzaldehyde is currently difficult to achieve with high benzyl alcohol conversion and high benzaldehyde selectivity simultaneously under mild conditions. Herein, the Fe-based catalysts anchored on nitrogen-doped carbon (x-Fe/NC) were prepared by thermal decomposition of the iron-doped zeolitic imidazolate framework precursors (x-Fe-ZIF). Among the various catalysts with different iron contents (x-Fe/NC), the 2-Fe/NC catalyst showed the best balance of conversion and selectivity, achieving 96.0% conversion of benzyl alcohol and around 98.0% selectivity for benzaldehyde. A range of characterization methods combined with kinetic analysis demonstrated that the high catalytic activity was attributed to the formed Fe–N_x active sites, which can accelerate the adsorption process of reactant molecules, facilitating the oxidation process while minimizing overoxidation to carboxylic acids. Moreover, the 2-Fe/NC catalyst showed excellent recyclability and substrate resistance, indicating its stability and potential for industrial application. This study offers fresh perspectives on the synthesis of effective transition metal-based catalysts and explores their potential applications in organic oxidation reactions.