NH3-SCR of NO over M/ZSM-5 (M = Mn, Co, Cu) catalysts: An in-situ DRIFTS study

被引:39
|
作者
Xue, Hongyan [1 ,2 ]
Guo, Xiaoming [2 ]
Meng, Tao [2 ]
Mao, Dongsen [2 ]
Ma, Zhen [1 ,3 ]
机构
[1] Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China
[2] Shanghai Inst Technol, Sch Chem & Environm Engn, Res Inst Appl Catalysis, Shanghai 201418, Peoples R China
[3] Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
关键词
ZSM-5; in-situ DRIFTS; Transition metal; NH3-SCR; Mechanism; LOW-TEMPERATURE; NITROGEN-OXIDES; METAL CU; FT-IR; REDUCTION; NH3; FE; MECHANISM; PERFORMANCE; CU-ZSM-5;
D O I
10.1016/j.surfin.2022.101722
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
M/ZSM-5 (M = Mn, Co, Cu) samples were prepared by impregnation, and the catalytic performance of these samples in NH3-SCR of NO was tested at 150-400 degrees C. Cu/ZSM-5 was more active than Mn/ZSM-5, and Co/ZSM-5 was the least active in NH3-SCR of NO. The nature and evolution of surface species were probed by in-situ DRIFTS. Among NH3-derived adsorbed species, coordinated NH3, NH4+, and amide (-NH2) species were found to be relevant for NH3-SCR. Among NOx-derived adsorbed species, bridged nitrate was the main active species. Bridged nitrate existed in larger quantities and was thermally more stable on Cu/ZSM-5 than on Mn/ZSM-5 and Co/ZSM-5, in line with the highest activity of Cu/ZSM-5. On the other hand, bidentate nitrate was inert towards NH3-SCR at low temperatures, whereas it became active at high temperatures. Both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms were applicable to Mn/Z at 150 degrees C, but only E-R mechanism was identified over Mn/Z at 300 degrees C. As for Co/Z and Cu/Z, both pathways existed simultaneously at 150 and 300 degrees C.
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页数:10
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