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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
来源:
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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