Journal
ACS CATALYSIS
Volume 10, Issue 3, Pages 2334-2344Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b05151
Keywords
NH3-SCR; AFX zeolite; kinetics study; in situ/operando IR; DFT calculation
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Funding
- Japan Ministry of Economy, Trade and Industry
- JST-CREST [JPMJCR17J3]
- JSPS KAKENHI [17H01341, 18K14057, 18K14051]
- MEXT project Elements Strategy Initiative to Form Core Research Centers [JPMXP0112101003]
- IRCCS
- JSPS [P19059]
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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.
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