▎ 摘　　要

Iron-based particles loaded on porous carbon materials have attracted extensive attention as catalysts for denitration and desulfurization reactions. However, the carbon support of a high-temperature denitration catalyst is inevitably oxidized in the presence of H2O and O-2. The mechanism of denitration catalyst oxidation and its influence on the catalytic reaction remain to be further explored. Fe2O3-loaded graphene models with carbon vacancy (G(def)), hydroxyl (HyG), and carboxyl (CyG) were constructed to investigate the effects of hydroxylation and carboxylation on the catalytic activity of Fe2O3/graphene for oxidative desulfurization and denitration by using density functional theory (DFT) calculations. According to the analysis of structural properties and adsorption energy, the adsorption process of Fe2O3 on HyG and CyG was observed to have proceeded more favorably than that on G(def). The density-of-states (DOS) results also affirmed that HyG and CyG promote the electron delocalization of Fe2O3 around the Fermi level, enhancing the chemical activity of Fe2O3. Moreover, adsorption energy analysis indicates that hydroxylation and carboxylation enhanced the adsorption of SO2 and H2O2 on Fe2O3/graphene while also maintaining preferable adsorption stability of NO. Furthermore, mechanistic research explains that adsorbed H2O2 on HyG and CyG directly oxidizes NO and SO2 into HNO2 and H2SO4 following a one-step reaction. The results provide a fundamental understanding of the oxidized catalyst on catalytic denitration and desulfurization reactions.