Insight into the origin of sulfur tolerance of Ag/Al2O3 in the H-2-C3H6-SCR of NOx
Xu, Guangyan; Ma, Jinzhu; Wang, Lian; Xie, Wen; Liu, Jingjing; Yu, Yunbo; He, Hong
刊名APPLIED CATALYSIS B-ENVIRONMENTAL
2019-05-05
卷号244页码:909-918
关键词HC-SCR Ag/Al2O3 Sulfur tolerance DRIFTS-MS DFT calculations
ISSN号0926-3373
英文摘要The sulfur tolerance of Ag/Al2O3 catalysts in Hrassisted C3H6-SCR was investigated by UV vis, TPR, TPSR, DRIFTS-MS, and DFT calculations. Ag/Al2O3 with higher silver loadings exhibited better deNOx performance and sulfur tolerance, especially the 4% Ag/Al2O3 catalyst. UV-vis and H-2-TPR revealed that highly dispersed Ag+ cations were predominant on 2% Ag/Al2O3, while more metallic Ag clusters with large sizes were present on the 4% Ag/Al2O3. After exposure to SO2, large amounts of sulfates were adsorbed on the Ag sites and Al sites of the Ag/Al2O3 surface. The sulfates were reduced to H2S and SO2 in a reducing atmosphere, while they showed little decomposition under real SCR reaction conditions. DRIFTS-MS experiments showed that sulfate species transferred rapidly between Ag sites and Al sites on the Ag/Al2O3 catalysts with higher amounts of Ag clusters. DFT calculations revealed that Ag-1 cations show stronger affinity for sulfate species than Ag clusters, thus resulting in blockage by sulfates at the Ag-O-Al interface. Such blocking by sulfates suppressed the activation of C3H6 as well as the formation of -NCO species, and thus severely inhibited the deNOx performance of 2% Ag/Al2O3. In contrast, the rapid mobility of sulfate species on 4% Ag/Al2O3 made more active sites available for the formation of key intermediates of HC-SCR, finally contributing to its excellent sulfur tolerance.
内容类型期刊论文
源URL[http://ir.rcees.ac.cn/handle/311016/43261]  
专题生态环境研究中心_水污染控制实验室
作者单位1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China
2.Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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Xu, Guangyan,Ma, Jinzhu,Wang, Lian,et al. Insight into the origin of sulfur tolerance of Ag/Al2O3 in the H-2-C3H6-SCR of NOx[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,244:909-918.
APA Xu, Guangyan.,Ma, Jinzhu.,Wang, Lian.,Xie, Wen.,Liu, Jingjing.,...&He, Hong.(2019).Insight into the origin of sulfur tolerance of Ag/Al2O3 in the H-2-C3H6-SCR of NOx.APPLIED CATALYSIS B-ENVIRONMENTAL,244,909-918.
MLA Xu, Guangyan,et al."Insight into the origin of sulfur tolerance of Ag/Al2O3 in the H-2-C3H6-SCR of NOx".APPLIED CATALYSIS B-ENVIRONMENTAL 244(2019):909-918.
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