On the Nature of Nitrogen-Containing Groups in the SCR of NO Over Functionalized Activated Coke

Abstract

To improve the denitrification efficiency for the selective catalytic reduction of NO with NH3 in the flue gas purification process, a low-rank activated coke (AC) was treated with ammonia (NH3·H2O) solution or nitric acid (HNO3) solution to increase the content and type of nitrogen-containing functional groups, and then the role of nitrogen-containing functional groups in the reduction of NO was analyzed. The modified AC samples were characterized by N2 adsorption/desorption to determine the pore structures and by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy to detect the surface functional groups. After modification, the content of oxygen-containing functional groups on the AC surface increased, including quinone, lactone and carboxyl, which are favorable for SO2 adsorption. Meanwhile, the type and content of nitrogen-containing functional groups on the AC surface changed; these groups fall into two categories: active groups and non-active groups. Before and after the denitrification process, the regular changes in the content of active and non-active groups showed that the active groups with pyrrole-like or pyridine-like structures can promote NO adsorption and then strengthen the denitrification. On the other hand, active groups may be reduced by NH3 or oxidized by O2, referring to side reactions, to generate non-active groups such as nitro, nitrate, amine and imine. More importantly, the role of nitrogen-containing functional groups was identified in the denitrification process. This chemical modification method is effective for improving the performance of low-cost AC since the employed chemicals are commercially available.