The Role of H+- and Cu+‑Sites for N2O Formation during NH3‑SCR over Cu-CHA

• Published in: Journal of physical chemistry. C Vol. 125; no. 8; pp. 4595 - 4601
• Main Authors: Feng, Yingxin, Janssens, Ton V. W, Vennestrøm, Peter N. R, Jansson, Jonas, Skoglundh, Magnus, Grönbeck, Henrik
• Format: Journal Article
• Language: English
• Published: American Chemical Society 04-03-2021
• Subjects: C: Chemical and Catalytic Reactivity at Interfaces; Cu-CHA; DFT; N2O; NH3-SCR
• ISSN: 1932-7447; 1932-7455; 1932-7455
• DOI: 10.1021/acs.jpcc.0c11008

The mechanism for N2O formation over CHA and Cu-CHA zeolite catalysts during NH3-SCR is investigated using density functional theory calculations. Direct NH4NO3 decomposition, which is commonly regarded as the main source of N2O, is found to be associated with high barriers in the absence of Brønsted acid sites. Although Brønsted acid sites promote NH4NO3 decomposition, it is still a highly activated process. Low-temperature N2O formation is instead found to be connected with an NO + NH3 reaction over Cu-sites. In particular, N2O can be formed from H2NNO with a low barrier over Cu-OOH-Cu complexes, which are proposed intermediates in the catalytic cycle for NH3-SCR over Cu-CHA. This finding provides an explanation for the experimentally observed low-temperature N2O formation and the relation between Cu loading and N2O formation. The proposed mechanisms open up strategies to enhance the selectivity to N2 during NH3-SCR.