Investigation on the catalytic roles of silver species in the selective catalytic reduction of NOx with methane

Abstract

Silver impregnated H-ZSM-5 zeolite catalysts with silver loading from 3 to 15wt.% were investigated for the selective catalytic reduction (SCR) of NOx with CH4 in the excess of oxygen. X-ray diffraction (XRD) and UV-Vis measurements established the structure of silver catalysts. A relationship between the structure of silver catalysts and their catalytic functions for the SCR of NOx by CH4 was clarified. The NO conversion to N2 showed a S-shape dependence on the increase of Ag loading. No linear dependence of catalytic activity on the amount of silver ions in the zeolite cation sites was observed. Contrastively, the activity was significantly enhanced by the nano-sized silver particles formed on the higher Ag loading samples (≥7wt.%). Temperature programmed desorption (TPD) and temperature programmed reduction (TPR) studies showed that nano-silver particles provided much stronger adsorption centers for active intermediates NO3−(s), on which adsorbed NO3−(s) could be effectively reduced by the activated methane. Silver ions in the zeolite cation sites might catalyze the reaction through activation of CH4 at lower temperatures. Activated CH4 reacted with NO3−(s) adsorbed on nano-silver particles to produce N2 and CO2.