Improvement of catalytic activity and sulfur-resistance of Ag/TiO₂–Al₂O₃ for NO reduction with propene under lean burn conditions

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• 作者：Junhua Li ; Yongqing Zhu ; Rui Ke ; Jiming Hao
• 关键词：Selective catalytic reduction of NO ; Ag/TiO₂– ; Al₂O₃ ; Activity enhancement ; SO₂ poisoning ; Lewis acid sites
• 刊名：Applied Catalysis B ; Environmental
• 出版年：2008
• 期刊代码：4_09263373
• 类别：ce
• 出版时间：8 May 2008
• 卷：80
• 期：3-4
• 页码：202-213
• 文件大小：1543 K

摘要

Ag-based catalysts supported on various metal oxides, Al₂O₃, TiO₂, and TiO₂–Al₂O₃, were prepared by the sol–gel method. The effect of SO₂ on catalytic activity was investigated for NO reduction with propene under lean burn condition. The results showed the catalytic activities were greatly enhanced on Ag/TiO₂–Al₂O₃ in comparison to Ag/Al₂O₃ and Ag/TiO₂, especially in the low temperature region. Application of different characterization techniques revealed that the activity enhancement was correlated with the properties of the support material. Silver was highly dispersed over the amorphous system of TiO₂–Al₂O₃. NO₃⁻ rather than NO₂⁻ or NOx reacted with the carboxylate species to form CN or NCO. NO₂ was the predominant desorption species in the temperature programmed desorption (TPD) of NO on Ag/TiO₂–Al₂O₃. More amount of formate (HCOO⁻) and CN were generated on the Ag/TiO₂–Al₂O₃ catalyst than the Ag/Al₂O₃ catalyst, due to an increased number of Lewis acid sites. Sulfate species, resulted from SO₂ oxidation, played dual roles on catalytic activity. On aged samples, the slow decomposition of accumulated sulfate species on catalyst surface led to poor NO conversion due to the blockage of these species on active sites. On the other hand, catalytic activity was greatly enhanced in the low temperature region because of the enhanced intensity of Lewis acid site caused by the adsorbed sulfate species. The rate of sulfate accumulation on the Ag/TiO₂–Al₂O₃ system was relatively slow. As a consequence, the system showed superior capability for selective adsorption of NO and SO₂ toleration to the Ag/Al₂O₃ catalyst.