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Formation and Reactions of NH4NO3 during Transient and Steady-State NH3-SCR of NOx, over H-AFX Zeolites: Spectroscopic and Theoretical Studies
| Title: | Formation and Reactions of NH4NO3 during Transient and Steady-State NH3-SCR of NOx, over H-AFX Zeolites: Spectroscopic and Theoretical Studies |
| Authors: | Kubota, Hiroe Browse this author | | Liu, Chong Browse this author | | Toyao, Takashi Browse this author →KAKEN DB | | Maeno, Zen Browse this author →KAKEN DB | | Ogura, Masaru Browse this author | | Nakazawa, Naoto Browse this author | | Inagaki, Satoshi Browse this author | | Kubota, Yoshihiro Browse this author | | Shimizu, Ken-ichi Browse this author →KAKEN DB |
| Keywords: | NH3-SCR | | AFX zeolite | | kinetics study | | in situ/operando IR | | DFT calculation |
| Issue Date: | 7-Feb-2020 |
| Publisher: | American Chemical Society |
| Journal Title: | ACS catalysis |
| Volume: | 10 |
| Issue: | 3 |
| Start Page: | 2334 |
| End Page: | 2344 |
| Publisher DOI: | 10.1021/acscatal.9b05151 |
| Abstract: | Operando infrared (IR) spectroscopy and density functional theory (DFT) calculations were combined to investigate the selective catalytic reduction (SCR) of NOx by NH3 over H-AFX zeolites. The steady-state kinetics shows that SCR reactions involving NO2 proceed much more rapidly than those of NO. Data from in situ IR combined with online mass spectrometry under transient conditions demonstrate that Bronsted acid sites (BASs) promote the reaction of NO2 with NH3 to form N-2, H2O, and NH4NO3 at low temperatures (50-150 degrees C). In combination with DFT results, these data suggest that NO promotes the reduction of NH4NO3 to NRINO2, which then decomposes into N-2 and H2O. Therefore, the accumulation of NH4NO3 in the zeolite is inhibited by NO. Furthermore, when NO is absent, NH4NO3 decomposition into N2O and H2O occurs only at high temperatures (>200 degrees C). A comparison of H-AFX and Cu-AFX implies that Cu sites are not active for the reduction of NO2 by NH3 and that BASs are responsible for the NH3-SCR reactions involving NO2. |
| Rights: | This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.9b05151 . |
| Type: | article (author version) |
| URI: | http://hdl.handle.net/2115/80393 |
| Appears in Collections: | 触媒科学研究所 (Institute for Catalysis) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)
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Submitter: 鳥屋尾 隆
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