Simultaneous removal of SO2 and NOx from flue gas using a CuO/Al2O3 catalyst sorbent II.: Promotion of SCR activity by SO2 at high temperatures

被引:138
作者
Xie, GY [1 ]
Liu, ZY [1 ]
Zhu, ZP [1 ]
Liu, QY [1 ]
Ge, J [1 ]
Huang, ZG [1 ]
机构
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
SO2; promoting effect; NOx; selective catalytic reduction (SCR); ammonia oxidation; CuO/Al2O3;
D O I
10.1016/j.jcat.2004.02.016
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
Promoting effect Of SO2 on selective catalytic reduction (SCR) of NO by NH3 over a CuO/Al2O3 catalyst sorbent has been investigated. Transient experiment, X-ray photoelectron spectroscopy (XPS), in situ DRIFT, NH3-TPD, and temperature-programmed reduction (TPR) were used to evaluate the promoting mechanism. The results show that the presence Of SO2 in the reaction stream can significantly promote catalytic activity of NO reduction at temperatures above 300 degreesC due to the formation of sulfate species on the catalyst surface. Sulfate species affect SCR activity by changing the acidity and redox property of the catalyst sorbent. In situ DRIFT shows that only ammonia coordinated on Lewis acid sites is found on the CuO/Al2O3 catalyst sorbent. Sulfation of CuO/Al2O3 catalyst sorbent greatly increases the concentration and strength of Lewis acid sites and the concentration of Bronsted acid sites. However, the ammonia bound to Bronsted acid sites does not play an important role in the SCR reaction in the catalyst system. Moreover, there is a close relationship between the SCR activity and ammonia oxidation activity. Ammonia oxidation experiments and TPR in H-2 suggest that sulfation of the catalyst sorbent weakens the catalyst's oxidation ability and inhibits NH3 oxidation to NO in the process of SCR, which may be another main promoting effect Of SO2 on SCR. (C) 2004 Elsevier Inc. All rights reserved.
引用
收藏
页码:42 / 49
页数:8
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