Enhanced CH3OH selectivity in CO2 hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites
Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual GaIII sites can be obtained via surface organometallic chemistry in a two-step process: (i) formation of isolated GaIII surface sites on SiO2 and (ii) subsequent grafting of a CuI prec...
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| Veröffentlicht in: | Chemical science (Cambridge) 2020-02, Vol.11 (29), p.7593-7598 |
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| creator | Lam, Erwin Noh, Gina Chan, Ka Wing Kim Larmier Lebedev, Dmitry Searles, Keith Wolf, Patrick Safonova, Olga V Copéret, Christophe |
| description | Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual GaIII sites can be obtained via surface organometallic chemistry in a two-step process: (i) formation of isolated GaIII surface sites on SiO2 and (ii) subsequent grafting of a CuI precursor, [Cu(OtBu)]4, followed by a treatment under H2 to generate CuGax alloys. This material is highly active and selective for CO2 hydrogenation to CH3OH. In situ X-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu0. This CuGa material only stabilizes methoxy surface species while no formate is detected according to ex situ infrared and solid-state nuclear magnetic resonance spectroscopy. |
| doi_str_mv | 10.1039/d0sc00465k |
| format | Article |
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This material is highly active and selective for CO2 hydrogenation to CH3OH. In situ X-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu0. This CuGa material only stabilizes methoxy surface species while no formate is detected according to ex situ infrared and solid-state nuclear magnetic resonance spectroscopy.</description><identifier>ISSN: 2041-6520</identifier><identifier>EISSN: 2041-6539</identifier><identifier>DOI: 10.1039/d0sc00465k</identifier><identifier>PMID: 34094136</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Alloying ; Carbon dioxide ; Chemistry ; Copper ; Gallium ; Hydrogenation ; Nanoalloys ; Nanoparticles ; NMR ; Nuclear magnetic resonance ; Organometallic compounds ; Selectivity ; Silicon dioxide ; X ray absorption</subject><ispartof>Chemical science (Cambridge), 2020-02, Vol.11 (29), p.7593-7598</ispartof><rights>Copyright Royal Society of Chemistry 2020</rights><rights>This journal is © The Royal Society of Chemistry 2020 The Royal Society of Chemistry</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC8159433/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC8159433/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,723,776,780,860,881,27903,27904,53770,53772</link.rule.ids></links><search><creatorcontrib>Lam, Erwin</creatorcontrib><creatorcontrib>Noh, Gina</creatorcontrib><creatorcontrib>Chan, Ka Wing</creatorcontrib><creatorcontrib>Kim Larmier</creatorcontrib><creatorcontrib>Lebedev, Dmitry</creatorcontrib><creatorcontrib>Searles, Keith</creatorcontrib><creatorcontrib>Wolf, Patrick</creatorcontrib><creatorcontrib>Safonova, Olga V</creatorcontrib><creatorcontrib>Copéret, Christophe</creatorcontrib><title>Enhanced CH3OH selectivity in CO2 hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites</title><title>Chemical science (Cambridge)</title><description>Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual GaIII sites can be obtained via surface organometallic chemistry in a two-step process: (i) formation of isolated GaIII surface sites on SiO2 and (ii) subsequent grafting of a CuI precursor, [Cu(OtBu)]4, followed by a treatment under H2 to generate CuGax alloys. This material is highly active and selective for CO2 hydrogenation to CH3OH. In situ X-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu0. This CuGa material only stabilizes methoxy surface species while no formate is detected according to ex situ infrared and solid-state nuclear magnetic resonance spectroscopy.</description><subject>Alloying</subject><subject>Carbon dioxide</subject><subject>Chemistry</subject><subject>Copper</subject><subject>Gallium</subject><subject>Hydrogenation</subject><subject>Nanoalloys</subject><subject>Nanoparticles</subject><subject>NMR</subject><subject>Nuclear magnetic resonance</subject><subject>Organometallic compounds</subject><subject>Selectivity</subject><subject>Silicon dioxide</subject><subject>X ray absorption</subject><issn>2041-6520</issn><issn>2041-6539</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNpdj09Lw0AQxRdRVKoXP8GCFy_R3Z3Nn70IEtQWlB7Uc5gkk3bbdFOzm0K_vRGLoHN5w8x7P2YYu5LiVgowd7XwlRA6iddH7FwJLaMkBnP82ytxxi69X4mxAGSs0lN2BloYLSE5Z_7RLdFVVPN8CvMp99RSFezOhj23judzxZf7uu8W5DDYzvHBW7fg-RCV6MdUhQHbvQ-ejw7qMYyznUX-Nn_NedN3G_6Ms9mMf6dairwN5C_YSYOtp8uDTtjH0-N7Po1e5s-z_OEl2o5nrqMkrRpJqHWpwaQaTQZYqjoDMAlVZaIFkapjLVFkTaNRyiaVRiBiU0rICCbs_oe7HcoN1RW50GNbbHu7wX5fdGiLvxtnl8Wi2xWZjI0GGAE3B0DffQ7kQ7GxvqK2RUfd4AsVQyZiSEedsOt_1lU39G58r1BaZcLIVMfwBdVPg2I</recordid><startdate>20200226</startdate><enddate>20200226</enddate><creator>Lam, Erwin</creator><creator>Noh, Gina</creator><creator>Chan, Ka Wing</creator><creator>Kim Larmier</creator><creator>Lebedev, Dmitry</creator><creator>Searles, Keith</creator><creator>Wolf, Patrick</creator><creator>Safonova, Olga V</creator><creator>Copéret, Christophe</creator><general>Royal Society of Chemistry</general><general>The Royal Society of Chemistry</general><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>7X8</scope><scope>5PM</scope></search><sort><creationdate>20200226</creationdate><title>Enhanced CH3OH selectivity in CO2 hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites</title><author>Lam, Erwin ; Noh, Gina ; Chan, Ka Wing ; Kim Larmier ; Lebedev, Dmitry ; Searles, Keith ; Wolf, Patrick ; Safonova, Olga V ; Copéret, Christophe</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p152k-67cf1ea44b43974a983ab2d83396ecb640ee2d541a08ff4a11f7190aaafb138e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Alloying</topic><topic>Carbon dioxide</topic><topic>Chemistry</topic><topic>Copper</topic><topic>Gallium</topic><topic>Hydrogenation</topic><topic>Nanoalloys</topic><topic>Nanoparticles</topic><topic>NMR</topic><topic>Nuclear magnetic resonance</topic><topic>Organometallic compounds</topic><topic>Selectivity</topic><topic>Silicon dioxide</topic><topic>X ray absorption</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lam, Erwin</creatorcontrib><creatorcontrib>Noh, Gina</creatorcontrib><creatorcontrib>Chan, Ka Wing</creatorcontrib><creatorcontrib>Kim Larmier</creatorcontrib><creatorcontrib>Lebedev, Dmitry</creatorcontrib><creatorcontrib>Searles, Keith</creatorcontrib><creatorcontrib>Wolf, Patrick</creatorcontrib><creatorcontrib>Safonova, Olga V</creatorcontrib><creatorcontrib>Copéret, Christophe</creatorcontrib><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Chemical science (Cambridge)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lam, Erwin</au><au>Noh, Gina</au><au>Chan, Ka Wing</au><au>Kim Larmier</au><au>Lebedev, Dmitry</au><au>Searles, Keith</au><au>Wolf, Patrick</au><au>Safonova, Olga V</au><au>Copéret, Christophe</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Enhanced CH3OH selectivity in CO2 hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites</atitle><jtitle>Chemical science (Cambridge)</jtitle><date>2020-02-26</date><risdate>2020</risdate><volume>11</volume><issue>29</issue><spage>7593</spage><epage>7598</epage><pages>7593-7598</pages><issn>2041-6520</issn><eissn>2041-6539</eissn><abstract>Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual GaIII sites can be obtained via surface organometallic chemistry in a two-step process: (i) formation of isolated GaIII surface sites on SiO2 and (ii) subsequent grafting of a CuI precursor, [Cu(OtBu)]4, followed by a treatment under H2 to generate CuGax alloys. This material is highly active and selective for CO2 hydrogenation to CH3OH. In situ X-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu0. This CuGa material only stabilizes methoxy surface species while no formate is detected according to ex situ infrared and solid-state nuclear magnetic resonance spectroscopy.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><pmid>34094136</pmid><doi>10.1039/d0sc00465k</doi><tpages>6</tpages><oa>free_for_read</oa></addata></record> |
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| source | DOAJ Directory of Open Access Journals; PubMed Central Open Access; EZB-FREE-00999 freely available EZB journals; PubMed Central |
| subjects | Alloying Carbon dioxide Chemistry Copper Gallium Hydrogenation Nanoalloys Nanoparticles NMR Nuclear magnetic resonance Organometallic compounds Selectivity Silicon dioxide X ray absorption |
| title | Enhanced CH3OH selectivity in CO2 hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites |
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