Insight into the H2S selective catalytic oxidation performance on well-mixed Ce-containing rare earth catalysts derived from MgAlCe layered double hydroxides

被引:49
|
作者
Zhang, Fenglian [1 ,2 ]
Zhang, Xin [1 ,2 ]
Hao, Zhengping [1 ,2 ]
Jiang, Guoxia [1 ,2 ]
Yang, Hongling [1 ,2 ]
Qu, Siqiu [3 ]
机构
[1] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Dept Environm Nanomat, Beijing 100085, Peoples R China
[2] Univ Chinese Acad Sci, Natl Engn Lab VOCs Pollut Control Mat & Technol, Beijing 101408, Peoples R China
[3] Shandong Sunway Petrochem Engn Share Co Ltd, Ctr Res & Dev, Beijing 100015, Peoples R China
关键词
Layered double hydroxides; Rare earth catalysts; H2S selective oxidation; Water effect; Catalytic mechanism; HYDROGEN-SULFIDE; ELEMENTAL SULFUR; CHEMICAL-COMPOSITION; TRANSITION-METAL; RAMAN-SPECTRA; SOLID BASE; OXIDES; CERIA; TEMPERATURE; MECHANISM;
D O I
10.1016/j.jhazmat.2017.09.014
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A series of well-mixed Ce-containing MgAlCe rare earth catalysts derived from layered double hydroxides were synthesized and tested for H2S selective catalytic oxidation. Particularly, no chemisorption O-vacancies but intrinsic defect sites were present on catalyst surface. Significantly, the catalysts exhibited excellent catalytic activity, reasonable durability, and outstanding sulfur selectivity (100%) at relatively low temperatures. Furthermore, the catalyst followed a step-wise mechanism, and the catalyst deactivation was due mainly to the slower oxidation rate of Ce3+ to Ce4+ by O-2 as compared to the reduction rate of Ce4+ to Ce3+ by H2S. Particularly, the added water, a Lewis base, can compete with inefficient S-8 catalyst for the occupation of Lewis acid sites and active sites. Meanwhile, it can change the characteristics of catalyst surface, resulting in sulfur existing form transforming from inefficient S-8 catalyst to inactive S3. Thus, lead to a decrease of deposited inefficient S-8 catalyst content. Consequently, decrease the catalytic activity. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:749 / 757
页数:9
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