Promotion effect of nitrogen doping on the low-temperature NH3-SCR of NO over activated carbon: Characterization and mechanism analysis

Abstract

Heteroatom nitrogen doping in carbon catalysts is recognized an effective strategy for tailoring the properties of carbon catalysts for various flue gas de-NOx applications. However, accurately discerning the active structures after nitrogen doping and elucidating the promotion effect on low-temperature selective catalytic reduction activity remains a formidable challenge under different nitrogen doping preparation conditions. In this study, a series of nitrogen-doped activated carbon catalysts was synthesized through the L16(45) orthogonal array design method, and the degree of influence of various preparation conditions on de-NOx catalytic activities was also assessed. The optimal preparation conditions determined by range analysis were employed to synthesize NOAC-17, achieving the NO conversion of 95% and N2 selectivity of 99% at 300 °C, respectively. Subsequently, various characterization results proved that nitrogen doping induced the formation of abundant basic groups. The imine, amide, amine, and N-6 groups altered the acid-base of the activated carbon surface and increased the adsorption of acidic NOx. The N-5 and N-Q groups enhanced electronic interaction in the carbon matrix and accelerated electron mobility in the catalytic reaction process. Moreover, the N-6 group played multiple roles beyond the aforementioned effect due to its special structure. It also enhanced the accumulation of oxygen vacancies, which were closely associated with further oxidation of adsorbed NO. The lone electron pair in the N-6 group within the activated carbon framework can alter the polarity of the catalyst, thereby exerting a positive influence on the adsorption and activation of NH3. The nitrogen-doped catalyst identified through range analysis of the orthogonal experiment primarily facilitated the NH3-SCR reaction via the E-R mechanism with supplementary contribution from L-H mechanism at low temperatures. The nitrogen doping conditions obtained for the activated carbon catalyst provide valuable insights for the strategic enhancement of its catalytic performance in low-temperature NH3-SCR reactions.