Citation: 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. doi: S1872-2067(19)63328-0 shu

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

State Key Laboratory of Silicon Materials and Center of Electron Microscopy, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China

Received Date: 14 January 2019
Revised Date: 19 February 2019

Fund Project: The authors acknowledge the support of the National Key Research and Development Program of China (2017YFB0310403), the National Natural Science Foundation of China (51872260, 51390474, 91645103), the Ministry of Science and Technology of China (2016YFE0105700), the Environmentally Sustainable Management of Medical Wastes in China (C/V/S/10/251), and the Zhejiang Provincial Natural Science Foundation of China (Z4080070, LD19B030001).

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.
- N₂O formation,
- NO reduction,
- Pd/CeO₂ catalyst,
- in-situ IR spectroscopy,
- Mechanism
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Mechanistic insight into N₂O formation during NO reduction by NH₃ over Pd/CeO₂ catalyst in the absence of O₂