Mechanistic insights into the enhanced low-temperature activity of Cu-SSZ-13 by MnOx-CeO2 modification for standard SCR reaction and fast SCR reactions

被引:1
|
作者
Li, Rui [1 ]
Yue, Tao [1 ]
Zheng, Yang [1 ]
Li, Guoliang [1 ]
Gao, Jiajia [1 ]
Zhang, Wenbo [1 ]
Wang, Jiaqing [1 ]
Ma, Mengying [1 ]
Su, Wei [1 ]
机构
[1] Univ Sci & Technol Beijing, Sch Energy & Environm Engn, Beijing 100083, Peoples R China
基金
中国国家自然科学基金;
关键词
Low-temperatureNH3-SCR; MnOx-CeO2/Cu-SSZ-13; Fast SCR reaction; Synergistic interaction; Reaction pathway; SELECTIVE CATALYTIC-REDUCTION; HYDROTHERMAL STABILITY; NH3-SCR; NO; PERFORMANCE; OXIDATION; ZEOLITE; NH3; OXIDES; MNOX;
D O I
10.1016/j.fuel.2024.131747
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Cu-SSZ-13 has been commercially utilized as NH 3 -SCR catalyst for diesel vehicles, yet its performance is hindered at low-temperatures and further inhibited by NO 2 . These issues could be mitigated by MnO x -CeO 2 modification, but the specific roles of MnO x and CeO 2 remained unclear. Through a combination of characterization methods, TPD/TPSR and DRIFTS, a promotional mechanism was proposed. In the standard SCR reaction, MnO x and CeO 2 modification facilitated NO oxidative activation by reducible Mn species and active oxygen species, promoting the L -H pathway by nitrite/nitrate species reacting with adsorbed NH 3 species. MnO x modification proved particularly effective for NO oxidative activation, generating monodentate nitrate and nitrite as active intermediates, thereby contributing to the superior low-temperature activity. Although the MnO x and CeO 2 modification also reduced high-temperature activity of Cu-SSZ-13, the MnO x -CeO 2 modification maintained high-temperature activity of Cu-SSZ-13 owing to the synergistic interaction between MnO x and CeO 2 on Cu-SSZ13. In the fast SCR reaction, MnO x modification promoted the reduction of NH 4 NO 3 and inhibited N 2 O release by producing bidentate nitrate and monodentate nitrate, and CeO 2 modification enhanced the reactivity and instability of NH 4 NO 3 , mitigating NH 4 NO 3 inhibition on NO reduction. This work provided an improved understanding of the standard SCR and fast SCR reactions of Cu-SSZ-13-based catalysts at low temperatures.
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页数:14
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