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Mechanistic insight into N_2O formation during NO reduction by NH_3 over pd/ceo_2 catalyst in the absence of O_2

Chinese Journal of Catalysis 2019年第7期40卷 1070-1077页

作者： Liping Sheng Zhaoxia Ma Shiyuan Chen Jinze Lou Chengye Li Songda Li Ze Zhang Yong Wang Hangsheng Yang State Key Laboratory of Silicon Materials and Center of Electron Microscopy School of Materials Science and EngineeringZhejiang UniversityHangzhou310027ZhejiangChina

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 N2 O emission during low-temperature NH3-SCR.

关键词： N2O formation NO reduction pd/ceo2 catalyst in-situ IR spectroscopy Mechanism

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