Acidity-activity correlation over bimetallic iron-based ZSM-5 catalysts during selective catalytic reduction of NO by NH3

被引:32
|
作者
Begum, Sayeda Halima [1 ,2 ,6 ]
Hung, Chin-Te [1 ]
Chen, Yit-Tsong [1 ,2 ]
Huang, Shing-Jong [3 ]
Wu, Pei-Hao [1 ]
Han, Xiaoxiang [4 ]
Liu, Shang-Bin [1 ,5 ]
机构
[1] Acad Sinica, Inst Atom & Mol Sci, Taipei 10617, Taiwan
[2] Natl Taiwan Univ, Dept Chem, Taipei 10617, Taiwan
[3] Natl Taiwan Univ, Instrumentat Ctr, Taipei 10617, Taiwan
[4] Zhejiang Gongshang Univ, Dept Appl Chem, Hangzhou 310035, Zhejiang, Peoples R China
[5] Natl Taiwan Normal Univ, Dept Chem, Taipei 11677, Taiwan
[6] Univ Chittagong, Dept Chem, Chittagong 4331, Bangladesh
关键词
Bimetallic Fe-based zeolite; Acidity; NOx reduction; NH3-SCR; P-31 MAS NMR; TEMPERATURE-PROGRAMMED DESORPTION; SOLID-STATE NMR; NITRIC-OXIDE; DENO(X) CATALYSTS; ZEOLITE CATALYSTS; SURFACE-ACIDITY; CHEMICAL-SHIFT; P-31; NMR; AMMONIA; SITES;
D O I
10.1016/j.molcata.2016.07.036
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
The effect of acidic properties over a series of Lanthanide metal incorporated Fe-based H-ZSM-5 (Si/Al = 15) catalysts on catalytic activity during selective catalytic reduction (SCR) of NO by NH3 was investigated. Various mono- (M-1-ZSM-5; M-1 = Fe, Ce, Pr, Nd, and Sm) and bimetallic (M2Fe-ZSM-5; M-2 = Ce, Pr, Nd, and Sm) catalysts were prepared and their physicochemical properties were characterized by a variety of analytical and spectroscopic techniques. In particular, their acidic properties were studied by different molecular probe techniques, including the conventional ammonia-TPD and pyridine-IR methods, as well as solid-state P-31 MAS NMR of adsorbed trimethylphosphine oxide (TMPO). Among various catalysts examined, the CeFe-ZSM-5 catalyst was found to exhibit an optimal NO conversion exceeding 95% over a temperature range of 300-500 degrees C (WHSV = 68,000 cm(3) g(-1) h(-1)). The superior SCR activity observed for the bimetallic Fe-based catalysts is attributed to the synergistic effect from the Bronsted acidity of the MFI zeolite and strong Lewis acidity induced by the incorporated active metal ion species, particularly when incorporated with a secondary Lanthanide metal ion. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:423 / 432
页数:10
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