In situ DRIFTS study and mechanism analysis of selective catalytic reduction of NOx by NH3 over ions doping MnCeOx/GR catalyst

Abstract

The present study demonstrates an innovative approach of doping MnCeOx/GR catalyst with three transition metal ions, namely Fe3+, Co3+, and Ni2+. Subsequently, the catalyst exhibiting superior performance was carefully selected. Meanwhile, the micro-reaction process of MnCeOx/GR and ion-doped MnCeOx/GR catalysts were established by in situ DRIFTS. The phenomena occurred in the experiment process were thoroughly examined through the application of various characteristic analysis, for instance, XRD, Raman, BET, XPS, H2-TPR, and NH3-TPD to analyze that Co3+ doping had a good improvement of activity and N2 selectivity on MnCeOx/GR catalyst at low temperature. This was evidenced by the activity test experiments, which revealed that CoMnCeOx/GR catalyst has the highest NO conversion within 150–225 °C temperature range, surpassing 90 %. Our findings showed that Co3+ doping not only enhanced redox capability and surface acidity, but also raised the relative Mn4+, Ce3+, and Oα content compared to MnCeOx/GR catalyst, which eventually contributed that the reactant molecules can be more effectively adsorbed onto the catalyst, thereby enhancing activation of NH3 and O2, thus improving efficiency of CoMnCeOx/GR catalyst. Additionally, it was proved that the Eley-Rideal and Langmuir-Hinshelwood mechanisms co-existed on CoMnCeOx/GR catalyst in a competitive way by in situ DRIFTS test.