Effect of doping Cr on NH3 adsorption and NO oxidation over the FexOy/AC surface: a DFT-D study

Abstract Activated carbon supported iron-based catalysts (FexOy/AC) show good deNOx efficiency at low temperature. The doping of chromium (Cr) greatly improves the catalyst activity. However, the detailed effect of doping Cr over FexOy/AC surface at molecular level is still a grey area. In this study, the roles of Cr dopant on gas adsorption and NO oxidation were deeply investigated by a DFT-D3 method. Results show that the synergy of Cr-Fe bimetal improves the binding capacity of Fe2O3/AC and Fe3O4/AC surface after doping Cr. NH3 can be adsorbed on Cr and Fe sites to form coordinated NH3. Doping Cr greatly improves the NH3 adsorption property on the Fe3O4/AC surface. NO molecule can combine with Cr, Fe, and O sites to form nitrosyl and nitrite. The doping of Cr increases the adsorption performance of NO on the Fe2O3/AC and Fe3O4/AC surfaces, especially for Fe3O4/AC surface. Furthermore, NO can be oxidized to NO2 by adsorption oxygen or active O sites of FexOy clusters. The doping of Cr restrains the formation of insoluble chelating bidentate nitrates and greatly reduces the reaction energy barrier of NO oxidation on the FexOy/AC surface, which can promote the deNOx reaction.