Mechanistic insight into N2O formation during NO reduction by NH3 over Pd/CeO2 catalyst in the absence of O2

doi:10.1016/S1872-2067(19)63328-0

Abstract

Abstract:

N₂O is a major by-product emitted during low-temperature selective catalytic reduction of NO with NH₃ (NH₃-SCR), which causes a series of serious environmental problems. A full understanding of the N₂O formation mechanism is essential to suppress the N₂O emission during the low-temperature NH₃-SCR, and requires an intensive study of this heterogeneous catalysis process. In this study, we investigated the reaction between NH₃ and NO over a Pd/CeO₂ catalyst in the absence of O₂, using X-ray photoelectron spectroscopy, NH₃-temperature-programmed desorption, NO-temperature-programmed desorption, and in-situ Fourier-transform infrared spectroscopy. Our results indicate that the N₂O formation mechanism is reaction-temperature-dependent. At temperatures below 250℃, the dissociation of HON, which is produced from the reaction between surface H·adatoms and adsorbed NO, is the key process for N₂O formation. At temperatures above 250℃, the reaction between NO and surface N·, which is produced by NO dissociation, is the only route for N₂O formation, and the dissociation of NO is the rate-determining step. Under optimal reaction conditions, a high performance with nearly 100% NO conversion and 100% N₂ selectivity could be achieved. These results provide important information to clarify the mechanism of N₂O formation and possible suppression of N₂O emission during low-temperature NH₃-SCR.

Key words: N₂O formation, NO reduction, Pd/CeO₂ catalyst, in-situ IR spectroscopy, Mechanism

Liping Sheng, Zhaoxia Ma, Shiyuan Chen, Jinze Lou, Chengye Li, Songda Li, Ze Zhang, Yong Wang, Hangsheng Yang. Mechanistic insight into N₂O formation during NO reduction by NH₃ over Pd/CeO₂ catalyst in the absence of O₂[J]. Chinese Journal of Catalysis, 2019, 40(7): 1070-1077.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(19)63328-0

https://www.cjcatal.com/EN/Y2019/V40/I7/1070

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Mechanistic insight into N₂O formation during NO reduction by NH₃ over Pd/CeO₂ catalyst in the absence of O₂

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