Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect
SBA-15 with varied pore size from 4 to 8 nm were synthesized by tuning the temperature of hydrothermal treatment, the supports were then used to load the active phase CrOx through a conventional impregnation method. The resulting catalysts were characterized by small/wide angle XRD, N2 adsorption/de...
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Veröffentlicht in: | Chinese journal of chemical engineering 2021-06, Vol.34 (6), p.77-86 |
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creator | Deng, Zhibin Ge, Xing Zhang, Wenting Luo, Shizhong Shen, Jun Jing, Fangli Chu, Wei |
description | SBA-15 with varied pore size from 4 to 8 nm were synthesized by tuning the temperature of hydrothermal treatment, the supports were then used to load the active phase CrOx through a conventional impregnation method. The resulting catalysts were characterized by small/wide angle XRD, N2 adsorption/desorption, FT-IR, TEM-EDX, XPS, TPR and CO2-TPD to study the feature of structure, surface chemical state, redox and basicity. It was found from these results that the metal species could be well dispersed on catalysts with larger pore size. Cr6+ species could enter into the framework by substituting the Si atoms of SBA-15, and Cr3+ mainly exist on extra framework. Pore size had profound effects on reducibility, surface composition and basicity. Cr6+ species were necessary to activate the C-H bonds of alkanes, while the basicity played an important role in activating C-O bonds of CO2. The best performances were achieved over the sample Cr supported on SBA-15 with a pore diameter of 7 nm in oxidative dehydrogenation of ethane in the presence of CO2.
[Display omitted]
•Pore size of SBA-15 was tuned by changing hydrothermal temperature.•Cr6+ could enter the framework of SBA-15 by partially replacing Si atoms.•Cr6+ and Cr3+ species co-existed on extra framework of SBA-15.•Cr6+ species were important for activating alkane.•Activation of CO2 was related to basicity of catalysts. |
doi_str_mv | 10.1016/j.cjche.2020.08.006 |
format | Article |
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[Display omitted]
•Pore size of SBA-15 was tuned by changing hydrothermal temperature.•Cr6+ could enter the framework of SBA-15 by partially replacing Si atoms.•Cr6+ and Cr3+ species co-existed on extra framework of SBA-15.•Cr6+ species were important for activating alkane.•Activation of CO2 was related to basicity of catalysts.</description><identifier>ISSN: 1004-9541</identifier><identifier>EISSN: 2210-321X</identifier><identifier>DOI: 10.1016/j.cjche.2020.08.006</identifier><language>eng</language><publisher>Elsevier B.V</publisher><subject>Cr catalysts ; Ethylene ; Heterogeneous catalysis ; Pore size effect ; SBA-15</subject><ispartof>Chinese journal of chemical engineering, 2021-06, Vol.34 (6), p.77-86</ispartof><rights>2020 Elsevier B.V.</rights><rights>Copyright © Wanfang Data Co. Ltd. All Rights Reserved.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c333t-3c700ac5df27c255154843d750e529a85d99d284b3d2986dfd28ea83bee086693</citedby><cites>FETCH-LOGICAL-c333t-3c700ac5df27c255154843d750e529a85d99d284b3d2986dfd28ea83bee086693</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Uhttp://www.wanfangdata.com.cn/images/PeriodicalImages/cjce/cjce.jpg</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.cjche.2020.08.006$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3550,27924,27925,45995</link.rule.ids></links><search><creatorcontrib>Deng, Zhibin</creatorcontrib><creatorcontrib>Ge, Xing</creatorcontrib><creatorcontrib>Zhang, Wenting</creatorcontrib><creatorcontrib>Luo, Shizhong</creatorcontrib><creatorcontrib>Shen, Jun</creatorcontrib><creatorcontrib>Jing, Fangli</creatorcontrib><creatorcontrib>Chu, Wei</creatorcontrib><title>Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect</title><title>Chinese journal of chemical engineering</title><description>SBA-15 with varied pore size from 4 to 8 nm were synthesized by tuning the temperature of hydrothermal treatment, the supports were then used to load the active phase CrOx through a conventional impregnation method. The resulting catalysts were characterized by small/wide angle XRD, N2 adsorption/desorption, FT-IR, TEM-EDX, XPS, TPR and CO2-TPD to study the feature of structure, surface chemical state, redox and basicity. It was found from these results that the metal species could be well dispersed on catalysts with larger pore size. Cr6+ species could enter into the framework by substituting the Si atoms of SBA-15, and Cr3+ mainly exist on extra framework. Pore size had profound effects on reducibility, surface composition and basicity. Cr6+ species were necessary to activate the C-H bonds of alkanes, while the basicity played an important role in activating C-O bonds of CO2. The best performances were achieved over the sample Cr supported on SBA-15 with a pore diameter of 7 nm in oxidative dehydrogenation of ethane in the presence of CO2.
[Display omitted]
•Pore size of SBA-15 was tuned by changing hydrothermal temperature.•Cr6+ could enter the framework of SBA-15 by partially replacing Si atoms.•Cr6+ and Cr3+ species co-existed on extra framework of SBA-15.•Cr6+ species were important for activating alkane.•Activation of CO2 was related to basicity of catalysts.</description><subject>Cr catalysts</subject><subject>Ethylene</subject><subject>Heterogeneous catalysis</subject><subject>Pore size effect</subject><subject>SBA-15</subject><issn>1004-9541</issn><issn>2210-321X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp9kD1PwzAQhi0EEuXjF7B4YUw420nqIDEgxJdUCQaQ2CzXvhBHbVzZaUuZ-Om4LTPT6U7vc6d7CLlgkDNg1VWXm860mHPgkIPMAaoDMuKcQSY4-zgkIwZQZHVZsGNyEmMHKSiZHJGfly9n9eBWSC22Gxv8J_ap9z31DcWh1T3StRtaanSYpql1PhFI_QoDjW7mjKZzP0OznOntAFcYaVwuFj4MaKlpg5-75ZzuqHhNX33AFPtGik2DZjgjR42eRTz_q6fk_eH-7e4pm7w8Pt_dTjIjhBgyYcYA2pS24WPDy5KVhSyEHZeAJa-1LG1dWy6LqbC8lpVtUoNaiikiyKqqxSm53O9d677R_afq_DL06aJK6jCJY1ABg5QT-5wJPsaAjVoEN9dhoxiorWzVqZ1stZWtQKokO1E3ewrTCyuHQUXjsDdoXUhPKuvdv_wvXCyLKw</recordid><startdate>20210601</startdate><enddate>20210601</enddate><creator>Deng, Zhibin</creator><creator>Ge, Xing</creator><creator>Zhang, Wenting</creator><creator>Luo, Shizhong</creator><creator>Shen, Jun</creator><creator>Jing, Fangli</creator><creator>Chu, Wei</creator><general>Elsevier B.V</general><general>College of Civil Aviation Safety Engineering,Civil Aviation Flight University of China,Guanghan 618307,China%Sinopec Petroleum Exploration and Production Research Institute,Northwest Oilfield Branch,Urumqi 830011,China%School of Chemical Engineering,Sichuan University,Chengdu 610065,China</general><scope>AAYXX</scope><scope>CITATION</scope><scope>2B.</scope><scope>4A8</scope><scope>92I</scope><scope>93N</scope><scope>PSX</scope><scope>TCJ</scope></search><sort><creationdate>20210601</creationdate><title>Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect</title><author>Deng, Zhibin ; Ge, Xing ; Zhang, Wenting ; Luo, Shizhong ; Shen, Jun ; Jing, Fangli ; Chu, Wei</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c333t-3c700ac5df27c255154843d750e529a85d99d284b3d2986dfd28ea83bee086693</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Cr catalysts</topic><topic>Ethylene</topic><topic>Heterogeneous catalysis</topic><topic>Pore size effect</topic><topic>SBA-15</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Deng, Zhibin</creatorcontrib><creatorcontrib>Ge, Xing</creatorcontrib><creatorcontrib>Zhang, Wenting</creatorcontrib><creatorcontrib>Luo, Shizhong</creatorcontrib><creatorcontrib>Shen, Jun</creatorcontrib><creatorcontrib>Jing, Fangli</creatorcontrib><creatorcontrib>Chu, Wei</creatorcontrib><collection>CrossRef</collection><collection>Wanfang Data Journals - Hong Kong</collection><collection>WANFANG Data Centre</collection><collection>Wanfang Data Journals</collection><collection>万方数据期刊 - 香港版</collection><collection>China Online Journals (COJ)</collection><collection>China Online Journals (COJ)</collection><jtitle>Chinese journal of chemical engineering</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Deng, Zhibin</au><au>Ge, Xing</au><au>Zhang, Wenting</au><au>Luo, Shizhong</au><au>Shen, Jun</au><au>Jing, Fangli</au><au>Chu, Wei</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect</atitle><jtitle>Chinese journal of chemical engineering</jtitle><date>2021-06-01</date><risdate>2021</risdate><volume>34</volume><issue>6</issue><spage>77</spage><epage>86</epage><pages>77-86</pages><issn>1004-9541</issn><eissn>2210-321X</eissn><abstract>SBA-15 with varied pore size from 4 to 8 nm were synthesized by tuning the temperature of hydrothermal treatment, the supports were then used to load the active phase CrOx through a conventional impregnation method. The resulting catalysts were characterized by small/wide angle XRD, N2 adsorption/desorption, FT-IR, TEM-EDX, XPS, TPR and CO2-TPD to study the feature of structure, surface chemical state, redox and basicity. It was found from these results that the metal species could be well dispersed on catalysts with larger pore size. Cr6+ species could enter into the framework by substituting the Si atoms of SBA-15, and Cr3+ mainly exist on extra framework. Pore size had profound effects on reducibility, surface composition and basicity. Cr6+ species were necessary to activate the C-H bonds of alkanes, while the basicity played an important role in activating C-O bonds of CO2. The best performances were achieved over the sample Cr supported on SBA-15 with a pore diameter of 7 nm in oxidative dehydrogenation of ethane in the presence of CO2.
[Display omitted]
•Pore size of SBA-15 was tuned by changing hydrothermal temperature.•Cr6+ could enter the framework of SBA-15 by partially replacing Si atoms.•Cr6+ and Cr3+ species co-existed on extra framework of SBA-15.•Cr6+ species were important for activating alkane.•Activation of CO2 was related to basicity of catalysts.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.cjche.2020.08.006</doi><tpages>10</tpages></addata></record> |
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subjects | Cr catalysts Ethylene Heterogeneous catalysis Pore size effect SBA-15 |
title | Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect |
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