A novel high activity MnXFe3−XO4 spinel catalyst for selective catalytic reduction of NO using NH3 prepared by a short process from natural minerals for low-temperature sintering flue gas: Effect of X value on catalytic mechanism

The process of smelting and purifying the catalyst precursor salt from minerals is extremely complex, which directly leads to high catalyst costs and serious secondary pollution. In order to achieve energy saving and emission reduction in the catalyst preparation process, in-situ synthesis of catalyst materials from natural minerals is a new research direction. In this study, we firstly explored the optimal X value of MnXFe3-XO4 for the NH3 selective catalytic reduction of NO (NH3-SCR) reaction, i.e., the Mn, Fe ratio, and then prepared a novel highly active mineral-based pure phase MnXFe3-XO4 spinel NH3-SCR catalyst by natural ferromanganese ore fines with iron-red fines (Fe2O3) allotment through in situ solid-phase synthesis and magnetic separation methods according to this ratio. The results show that the X value of 1.5 (Mn1.5Fe1.5O4) is the best for NH3-SCR reaction. Mn1.5Fe1.5O4 nano-particles (201 nm) has nearly 100 % NO conversion (with 5 % H2O(g)) at 125–300 °C. The combination of characterizations and density functional theory (DFT) calculation shows that the catalytic process of Eley-Rideal (E-R) dehydrogenation is enhanced at both the active site Mn site and Fe site, which is a key factor in the acceleration of the NH3-SCR reaction with increasing X value at the MnXFe3-XO4 surface.