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- W3199498049 abstract "Toward the rational design of new lean NOx reduction catalysts under periodic lean (NO + O2) and rich (NO + H2) cycle conditions, we studied the reactions of adsorbed NO and NH3 on Rh-exchanged Al-rich (Si/Al = 5) beta zeolites (Rh4β5) under transient (lean ↔ rich) and temperature ramping conditions. In situ infrared (IR) spectra of adsorbed species were collected while monitoring the outlet gas by mass spectrometry (MS) and another IR gas cell, enabling an operando analysis of the surface reactions. Dynamic changes in the catalyst structure were studied by X-ray absorption spectroscopy (XAS), H2-temperature-programed reduction (TPR), and operando IR spectroscopy. Rh0 metal clusters, Rh+, and Rh3+ species were copresent in the catalyst after H2 reduction at 500 °C. Under NO or NO + O2 flow, the Rh+ site (NO storage site) in the reduced Rh4β5 captured NO in the form of [Rh(NO)2]+, which was stable under oxidative (lean) conditions. The captured NO was selectively reduced by H2 to NH3. The in-situ-generated NH3 was captured by a Brønsted acid site (NH3 storage site). The captured NH3 reduced NO to N2 in the next lean (NO + O2) period. Finally, Rh4β5 was applied to the lean de-NOx system under cyclic lean/rich conditions, accompanied by NOx reduction under periodic lean (0.1% NO + 2% O2)/rich (0.1% NO + 2% H2) cycles. The NOx trapped in the lean period is reduced to adsorbed NH3 in the rich period, which subsequently reduces NO to N2 in the next lean period." @default.
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- W3199498049 date "2021-09-20" @default.
- W3199498049 modified "2023-10-15" @default.
- W3199498049 title "Lean NO<i>x</i> Reduction by In-Situ-Formed NH<sub>3</sub> under Periodic Lean/Rich Conditions over Rhodium-Loaded Al-Rich Beta Zeolites" @default.
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- W3199498049 doi "https://doi.org/10.1021/acscatal.1c03396" @default.
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