On the selectively catalytic reduction of NOx with methane over Ag-ZSM-5 catalysts

Abstract

The catalytic performance of silver-modified ZSM-5 catalysts in the selectively catalytic reduction (SCR) of NOx with methane was investigated. NO was selectively reduced by CH4 to N2 in the presence of excess O2, and the catalytic activity depended on both the activation of CH4 and the adsorption properties of NOx. Silver incorporated in ZSM-5 zeolite activated CH4 at low temperatures and lowered the “light-off” temperature for the CH4-SCR of NOx. Temperature-programmed (TP) spectroscopy studies depicted that surface nitrosyl species directly decomposed to N2 in the absence of O2. CH4 could not effectively reduce surface nitrosyl species, but might facilitate the direct decomposition of NO through the removal of surface oxygen. Surface nitrates were formed in NO and O2 coexisting system and could be effectively reduced by CH4 to nitrogen. The priority of surface nitrates to O2 in the reaction with CH4 clearly demonstrated that CH4 selectively and preferentially reduced the surface nitrate species to N2 in the excess of oxygen.