Abstract
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 Bronsted acid sites. Although Bronsted 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.
Sign-in/Register to access full text options 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
