Low Temperature deNOx Catalytic Activity with C2H4 as a Reductant Using Mixed Metal Fe-Mn Oxides Supported on Activated Carbon

Abstract

The selective catalytic reduction of NOx (deNOx) at temperatures less than or at 200 °C was investigated while using C2H4 as the reductant and mixed oxides of Fe and Mn supported on activated carbon; their activity was compared to that of MnOx and FeOx separately supported on activated carbon. The bimetallic oxide compositions maintained high NO conversion of greater than 80–98% for periods that were three times greater than those of the supported monometallic oxides. To examine potential reasons for the significant increases in activity maintenance, and subsequent deactivation, the catalysts were examined by using bulk and surface sensitive analytical techniques before and after catalyst testing. No significant changes in Brunauer-Emmett-Teller (BET) surface areas or porosities were observed between freshly-prepared and tested catalysts whereas segregation of FeOx and MnOx species was readily observed in the mono-oxide catalysts after reaction testing that was not detected in the mixed oxide catalysts. Furthermore, x-ray diffraction and Raman spectroscopy data detected cubic Fe3Mn3O8 in both the freshly-prepared and reaction-tested mixed oxide catalysts that were more crystalline after testing. The presence of this compound, which is known to stabilize multivalent Fe species and to enhance oxygen transfer reactions, may be the reason for the high and relatively stable NO conversion activity, and its increased crystallinity during longer-term testing may also decrease surface availability of the active sites responsible for NO conversion. These results point to a potential of further enhancing catalyst stability and activity for low temperature deNOx that is applicable to advanced SCR processing with lower costs and less deleterious side effects to processing equipment.