Activated carbon catalyst for selective oxidation of hydrogen sulphide: On the influence of pore structure, surface characteristics, and catalytically-active nitrogen

被引:146
作者
Bashkova, Svetlana [1 ]
Baker, Frederick S. [1 ]
Wu, Xianxian [1 ]
Armstrong, Timothy R. [1 ]
Schwartz, Viviane [1 ]
机构
[1] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA
关键词
D O I
10.1016/j.carbon.2007.01.005
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 catalytic oxidation of hydrogen sulphide (H2S) on various activated carbon materials was studied. The effects of pore structure, surface characteristics, and nitrogen content on the activity and selectivity of the carbons towards oxidation of H2S were investigated. It was found that a high volume of both micropores and small mesopores, in combination with a relatively narrow pore size distribution, were crucial for the retention of sulphur dioxide (SO2) a by-product of H2S oxidation. For the retention of carbonyl sulphide (COS), another H2S oxidation by-product, high surface reactivity with a significant amount of basic groups were found to be important. The only carbon with all these characteristics, and consequently the carbon that was able to retain both H2S and COS for an extended period of time, was an experimental product, '' WSC ''. This carbon was found to be superior to the other carbons studied, exhibiting high activity and selectivity for oxidation of H2S to Sulphur. H2S breakthrough capacities and selectivity values of the carbons were found to be dependent on the nitrogen content of the carbons. In a hydrogen stream, carbons possessing the highest nitrogen contents exhibited the greatest H2S breakthrough capacities but, at the same time, the lowest selectivity with respect to sulphur formation. In reformate streams, the maximum breakthrough capacity and greatest selectivity were exhibited by carbons with a nitrogen content of about 1-1.5 wt%. (C) 2007 Elsevier Ltd. All rights reserved.
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页码:1354 / 1363
页数:10
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