Ruthenium nanoparticles supported on magnesium oxide: A versatile and recyclable dual-site catalyst for hydrogenation of mono- and poly-cyclic arenes, N-heteroaromatics, and S-heteroaromatics
[Display omitted] •The catalyst is prepared through a simple one-pot procedure at room temperature.•The catalyst hydrogenates mono-/poly-cyclic hydrocarbons and N/S-hetero aromatics.•The catalyst displays higher activity and broader scope than other supported metals.•The catalyst is not poisoned by...
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Veröffentlicht in: | Journal of catalysis 2014-03, Vol.311, p.357-368 |
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creator | Fang, Minfeng Sánchez-Delgado, Roberto A. |
description | [Display omitted]
•The catalyst is prepared through a simple one-pot procedure at room temperature.•The catalyst hydrogenates mono-/poly-cyclic hydrocarbons and N/S-hetero aromatics.•The catalyst displays higher activity and broader scope than other supported metals.•The catalyst is not poisoned by N/S heterocycles and is recyclable and long-lived.•A dual hydrogenation mechanism operating on two distinct active sites is proposed.
The development of catalysts capable of promoting hydrogenation of aromatics while being resistant to poisoning by nitrogen- and sulfur-containing species is of much interest in connection with hydrotreating of fossil fuels. We report a catalyst composed of ruthenium nanoparticles supported on magnesia, designed to promote heterolytic hydrogen splitting and surface ionic hydrogenation pathways. The catalyst, prepared through a one-pot procedure, promotes the hydrogenation of mono- and poly-cyclic arenes, as well as N- and S-heteroaromatics representative of fossil fuels components. Of particular significance are the superior activity and wider substrate scope of the catalyst, in relation to other known supported noble metals, and the excellent recyclability and long catalyst lifetime. Based on our experimental data, a dual-site catalyst structure and an associated dual-pathway mechanism are proposed, which may have interesting implications for the development of new poison-tolerant noble metal catalytic systems. |
doi_str_mv | 10.1016/j.jcat.2013.12.017 |
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•The catalyst is prepared through a simple one-pot procedure at room temperature.•The catalyst hydrogenates mono-/poly-cyclic hydrocarbons and N/S-hetero aromatics.•The catalyst displays higher activity and broader scope than other supported metals.•The catalyst is not poisoned by N/S heterocycles and is recyclable and long-lived.•A dual hydrogenation mechanism operating on two distinct active sites is proposed.
The development of catalysts capable of promoting hydrogenation of aromatics while being resistant to poisoning by nitrogen- and sulfur-containing species is of much interest in connection with hydrotreating of fossil fuels. We report a catalyst composed of ruthenium nanoparticles supported on magnesia, designed to promote heterolytic hydrogen splitting and surface ionic hydrogenation pathways. The catalyst, prepared through a one-pot procedure, promotes the hydrogenation of mono- and poly-cyclic arenes, as well as N- and S-heteroaromatics representative of fossil fuels components. Of particular significance are the superior activity and wider substrate scope of the catalyst, in relation to other known supported noble metals, and the excellent recyclability and long catalyst lifetime. Based on our experimental data, a dual-site catalyst structure and an associated dual-pathway mechanism are proposed, which may have interesting implications for the development of new poison-tolerant noble metal catalytic systems.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/j.jcat.2013.12.017</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>Aromatics ; Catalysis ; Catalysts ; Chemistry ; Colloidal state and disperse state ; Dual-site ; Exact sciences and technology ; General and physical chemistry ; Heterolytic hydrogen splitting ; Hydrogenation ; Ionic hydrogenation mechanism ; Magnesium ; Magnesium oxide ; N-heteroaromatics ; Nanoparticles ; Oxidation ; Physical and chemical studies. Granulometry. Electrokinetic phenomena ; Polycyclic aromatic hydrocarbons ; Ru nanoparticles ; S-heteroaromatics ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><ispartof>Journal of catalysis, 2014-03, Vol.311, p.357-368</ispartof><rights>2014 Elsevier Inc.</rights><rights>2015 INIST-CNRS</rights><rights>Copyright © 2014 Elsevier B.V. All rights reserved.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c395t-4e4ce8fb126ab726fae85ca80d509813eb911524515092d65dc3550164ca49ca3</citedby><cites>FETCH-LOGICAL-c395t-4e4ce8fb126ab726fae85ca80d509813eb911524515092d65dc3550164ca49ca3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.jcat.2013.12.017$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,778,782,3539,27907,27908,45978</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=28313082$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Fang, Minfeng</creatorcontrib><creatorcontrib>Sánchez-Delgado, Roberto A.</creatorcontrib><title>Ruthenium nanoparticles supported on magnesium oxide: A versatile and recyclable dual-site catalyst for hydrogenation of mono- and poly-cyclic arenes, N-heteroaromatics, and S-heteroaromatics</title><title>Journal of catalysis</title><description>[Display omitted]
•The catalyst is prepared through a simple one-pot procedure at room temperature.•The catalyst hydrogenates mono-/poly-cyclic hydrocarbons and N/S-hetero aromatics.•The catalyst displays higher activity and broader scope than other supported metals.•The catalyst is not poisoned by N/S heterocycles and is recyclable and long-lived.•A dual hydrogenation mechanism operating on two distinct active sites is proposed.
The development of catalysts capable of promoting hydrogenation of aromatics while being resistant to poisoning by nitrogen- and sulfur-containing species is of much interest in connection with hydrotreating of fossil fuels. We report a catalyst composed of ruthenium nanoparticles supported on magnesia, designed to promote heterolytic hydrogen splitting and surface ionic hydrogenation pathways. The catalyst, prepared through a one-pot procedure, promotes the hydrogenation of mono- and poly-cyclic arenes, as well as N- and S-heteroaromatics representative of fossil fuels components. Of particular significance are the superior activity and wider substrate scope of the catalyst, in relation to other known supported noble metals, and the excellent recyclability and long catalyst lifetime. Based on our experimental data, a dual-site catalyst structure and an associated dual-pathway mechanism are proposed, which may have interesting implications for the development of new poison-tolerant noble metal catalytic systems.</description><subject>Aromatics</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemistry</subject><subject>Colloidal state and disperse state</subject><subject>Dual-site</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Heterolytic hydrogen splitting</subject><subject>Hydrogenation</subject><subject>Ionic hydrogenation mechanism</subject><subject>Magnesium</subject><subject>Magnesium oxide</subject><subject>N-heteroaromatics</subject><subject>Nanoparticles</subject><subject>Oxidation</subject><subject>Physical and chemical studies. Granulometry. Electrokinetic phenomena</subject><subject>Polycyclic aromatic hydrocarbons</subject><subject>Ru nanoparticles</subject><subject>S-heteroaromatics</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><recordid>eNp9kcuO1DAQRSMEEs3AD7CyhNiRYDtxOkFsRiNe0ggkHmur2q5MO0rbwXZGk6_j16jQIxYsWFlVuqeqfG9RPBe8Ely0r8dqNJAryUVdCVlxsX9Q7ATveSnbvnlY7DiXouyV2D8unqQ0ci6EUt2u-PV1yUf0bjkxDz7MELMzEyaWlnkOMaNlwbMT3HhMmyjcOYtv2CW7xZgguwkZeMsimtVMcKDSLjCVyWVkdBFMa8psCJEdVxvDDXpiaGAY2Cn4UP6B5zCt5cY7wyAibXrFPpdHzBgDxHAixFBrk377t_20eDTAlPDZ_XtR_Hj_7vvVx_L6y4dPV5fXpal7lcsGG4PdcBCyhcNetgNgpwx03Cred6LGQ0-GyEYJqqVtlTW1UuRsY6DpDdQXxYvz3DmGnwumrMewRE8rNSHECNn1pJJnlYkhpYiDnqM7QVy14HoLSo96C0pvQWkhNQVF0Mv70ZAMTEMEb1z6S8quFjXvJOnennVI_7x1GHUyDr1B68j-rG1w_1vzGzuUrVg</recordid><startdate>20140301</startdate><enddate>20140301</enddate><creator>Fang, Minfeng</creator><creator>Sánchez-Delgado, Roberto A.</creator><general>Elsevier Inc</general><general>Elsevier</general><general>Elsevier BV</general><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20140301</creationdate><title>Ruthenium nanoparticles supported on magnesium oxide: A versatile and recyclable dual-site catalyst for hydrogenation of mono- and poly-cyclic arenes, N-heteroaromatics, and S-heteroaromatics</title><author>Fang, Minfeng ; Sánchez-Delgado, Roberto A.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c395t-4e4ce8fb126ab726fae85ca80d509813eb911524515092d65dc3550164ca49ca3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>Aromatics</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Chemistry</topic><topic>Colloidal state and disperse state</topic><topic>Dual-site</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>Heterolytic hydrogen splitting</topic><topic>Hydrogenation</topic><topic>Ionic hydrogenation mechanism</topic><topic>Magnesium</topic><topic>Magnesium oxide</topic><topic>N-heteroaromatics</topic><topic>Nanoparticles</topic><topic>Oxidation</topic><topic>Physical and chemical studies. Granulometry. Electrokinetic phenomena</topic><topic>Polycyclic aromatic hydrocarbons</topic><topic>Ru nanoparticles</topic><topic>S-heteroaromatics</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Fang, Minfeng</creatorcontrib><creatorcontrib>Sánchez-Delgado, Roberto A.</creatorcontrib><collection>Pascal-Francis</collection><collection>CrossRef</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Fang, Minfeng</au><au>Sánchez-Delgado, Roberto A.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Ruthenium nanoparticles supported on magnesium oxide: A versatile and recyclable dual-site catalyst for hydrogenation of mono- and poly-cyclic arenes, N-heteroaromatics, and S-heteroaromatics</atitle><jtitle>Journal of catalysis</jtitle><date>2014-03-01</date><risdate>2014</risdate><volume>311</volume><spage>357</spage><epage>368</epage><pages>357-368</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><coden>JCTLA5</coden><abstract>[Display omitted]
•The catalyst is prepared through a simple one-pot procedure at room temperature.•The catalyst hydrogenates mono-/poly-cyclic hydrocarbons and N/S-hetero aromatics.•The catalyst displays higher activity and broader scope than other supported metals.•The catalyst is not poisoned by N/S heterocycles and is recyclable and long-lived.•A dual hydrogenation mechanism operating on two distinct active sites is proposed.
The development of catalysts capable of promoting hydrogenation of aromatics while being resistant to poisoning by nitrogen- and sulfur-containing species is of much interest in connection with hydrotreating of fossil fuels. We report a catalyst composed of ruthenium nanoparticles supported on magnesia, designed to promote heterolytic hydrogen splitting and surface ionic hydrogenation pathways. The catalyst, prepared through a one-pot procedure, promotes the hydrogenation of mono- and poly-cyclic arenes, as well as N- and S-heteroaromatics representative of fossil fuels components. Of particular significance are the superior activity and wider substrate scope of the catalyst, in relation to other known supported noble metals, and the excellent recyclability and long catalyst lifetime. Based on our experimental data, a dual-site catalyst structure and an associated dual-pathway mechanism are proposed, which may have interesting implications for the development of new poison-tolerant noble metal catalytic systems.</abstract><cop>Amsterdam</cop><pub>Elsevier Inc</pub><doi>10.1016/j.jcat.2013.12.017</doi><tpages>12</tpages></addata></record> |
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subjects | Aromatics Catalysis Catalysts Chemistry Colloidal state and disperse state Dual-site Exact sciences and technology General and physical chemistry Heterolytic hydrogen splitting Hydrogenation Ionic hydrogenation mechanism Magnesium Magnesium oxide N-heteroaromatics Nanoparticles Oxidation Physical and chemical studies. Granulometry. Electrokinetic phenomena Polycyclic aromatic hydrocarbons Ru nanoparticles S-heteroaromatics Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry |
title | Ruthenium nanoparticles supported on magnesium oxide: A versatile and recyclable dual-site catalyst for hydrogenation of mono- and poly-cyclic arenes, N-heteroaromatics, and S-heteroaromatics |
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