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

[Display omitted] •The MgAlCeO rare earth catalysts exhibited excellent catalytic activities.•No chemisorption O vacancies existed on catalyst surface.•The MgAlCeO rare earth catalysts obeyed a step-wise mechanism.•The effect of added water was investigated deeply. A series of well-mixed Ce-containi...

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Veröffentlicht in:Journal of hazardous materials 2018-01, Vol.342, p.749-757
Hauptverfasser: Zhang, Fenglian, Zhang, Xin, Hao, Zhengping, Jiang, Guoxia, Yang, Hongling, Qu, Siqiu
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container_end_page 757
container_issue
container_start_page 749
container_title Journal of hazardous materials
container_volume 342
creator Zhang, Fenglian
Zhang, Xin
Hao, Zhengping
Jiang, Guoxia
Yang, Hongling
Qu, Siqiu
description [Display omitted] •The MgAlCeO rare earth catalysts exhibited excellent catalytic activities.•No chemisorption O vacancies existed on catalyst surface.•The MgAlCeO rare earth catalysts obeyed a step-wise mechanism.•The effect of added water was investigated deeply. 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 O2 as compared to the reduction rate of Ce4+ to Ce3+ by H2S. Particularly, the added water, a Lewis base, can compete with inefficient S8 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 S8 catalyst to inactive S3. Thus, lead to a decrease of deposited inefficient S8 catalyst content. Consequently, decrease the catalytic activity.
doi_str_mv 10.1016/j.jhazmat.2017.09.014
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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 O2 as compared to the reduction rate of Ce4+ to Ce3+ by H2S. Particularly, the added water, a Lewis base, can compete with inefficient S8 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 S8 catalyst to inactive S3. Thus, lead to a decrease of deposited inefficient S8 catalyst content. 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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 O2 as compared to the reduction rate of Ce4+ to Ce3+ by H2S. Particularly, the added water, a Lewis base, can compete with inefficient S8 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 S8 catalyst to inactive S3. Thus, lead to a decrease of deposited inefficient S8 catalyst content. Consequently, decrease the catalytic activity.</description><subject>Catalytic mechanism</subject><subject>H2S selective oxidation</subject><subject>Layered double hydroxides</subject><subject>Rare earth catalysts</subject><subject>Water effect</subject><issn>0304-3894</issn><issn>1873-3336</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNqFUcuO1DAQtBBIDAufgOQjlwQ77bxOaDWC3ZUWcQDOVsfuTDxK4sH2LDv8C_-KRzN3Tq1uVVWrqhh7L0UphWw-7sv9hH8WTGUlZFuKvhRSvWAb2bVQAEDzkm0ECFVA16vX7E2MeyEyslYb9vdhjW43Je7W5HmaiN9X33mkmUxyT8QNJpxPyRnun53F5PzKDxRGHxZcDfG8_qZ5Lhb3TJZvqTB-TehWt-54wECcMKTpKhNT5JZC1rV8DH7hX3e385b4jCcK-Wb9cZiJTycbzt8ovmWvRpwjvbvOG_bzy-cf2_vi8dvdw_b2sTDQ9qno-rqtBoROUdVIVE1LPTTV0MlR4CgA6sEIVGCtwhqawbRgOoCKjDVirEa4YR8uuofgfx0pJr24aLIvXMkfo5a9ErJvVNtmaH2BmuBjDDTqQ3ALhpOWQp_r0Ht9rUOf69Ci17mOzPt04VH28eQo6Ggc5QitCzlrbb37j8I_eBeZ7A</recordid><startdate>20180115</startdate><enddate>20180115</enddate><creator>Zhang, Fenglian</creator><creator>Zhang, Xin</creator><creator>Hao, Zhengping</creator><creator>Jiang, Guoxia</creator><creator>Yang, Hongling</creator><creator>Qu, Siqiu</creator><general>Elsevier B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20180115</creationdate><title>Insight into the H2S selective catalytic oxidation performance on well-mixed Ce-containing rare earth catalysts derived from MgAlCe layered double hydroxides</title><author>Zhang, Fenglian ; Zhang, Xin ; Hao, Zhengping ; Jiang, Guoxia ; Yang, Hongling ; Qu, Siqiu</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c379t-89572ba384e261a467e9362b81f0af0335bc0a43dd4a536bc73c8332ecdc0f2f3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Catalytic mechanism</topic><topic>H2S selective oxidation</topic><topic>Layered double hydroxides</topic><topic>Rare earth catalysts</topic><topic>Water effect</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Fenglian</creatorcontrib><creatorcontrib>Zhang, Xin</creatorcontrib><creatorcontrib>Hao, Zhengping</creatorcontrib><creatorcontrib>Jiang, Guoxia</creatorcontrib><creatorcontrib>Yang, Hongling</creatorcontrib><creatorcontrib>Qu, Siqiu</creatorcontrib><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Journal of hazardous materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Fenglian</au><au>Zhang, Xin</au><au>Hao, Zhengping</au><au>Jiang, Guoxia</au><au>Yang, Hongling</au><au>Qu, Siqiu</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Insight into the H2S selective catalytic oxidation performance on well-mixed Ce-containing rare earth catalysts derived from MgAlCe layered double hydroxides</atitle><jtitle>Journal of hazardous materials</jtitle><date>2018-01-15</date><risdate>2018</risdate><volume>342</volume><spage>749</spage><epage>757</epage><pages>749-757</pages><issn>0304-3894</issn><eissn>1873-3336</eissn><abstract>[Display omitted] •The MgAlCeO rare earth catalysts exhibited excellent catalytic activities.•No chemisorption O vacancies existed on catalyst surface.•The MgAlCeO rare earth catalysts obeyed a step-wise mechanism.•The effect of added water was investigated deeply. 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 O2 as compared to the reduction rate of Ce4+ to Ce3+ by H2S. Particularly, the added water, a Lewis base, can compete with inefficient S8 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 S8 catalyst to inactive S3. Thus, lead to a decrease of deposited inefficient S8 catalyst content. Consequently, decrease the catalytic activity.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.jhazmat.2017.09.014</doi><tpages>9</tpages></addata></record>
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subjects Catalytic mechanism
H2S selective oxidation
Layered double hydroxides
Rare earth catalysts
Water effect
title Insight into the H2S selective catalytic oxidation performance on well-mixed Ce-containing rare earth catalysts derived from MgAlCe layered double hydroxides
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