A Silicon-Heteroaromatic System as Photosensitizer for Light-Driven Hydrogen Production by Hydrogenase Mimics
The utilization of light and inexpensive catalysts to afford hydrogen represents a huge challenge. Following our interest in silicon‐containing [FeFe]‐hydrogenase ([FeFe]‐H2ase) mimics, we report a new model approach for a photocatalytic [FeFe]‐H2ase mimic 1, which contains a 1‐silafluorene unit as...
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| Veröffentlicht in: | European journal of inorganic chemistry 2013-09, Vol.2013 (25), p.4466-4472 |
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| container_title | European journal of inorganic chemistry |
| container_volume | 2013 |
| creator | Goy, Roman Apfel, Ulf-Peter Elleouet, Catherine Escudero, Daniel Elstner, Martin Görls, Helmar Talarmin, Jean Schollhammer, Philippe González, Leticia Weigand, Wolfgang |
| description | The utilization of light and inexpensive catalysts to afford hydrogen represents a huge challenge. Following our interest in silicon‐containing [FeFe]‐hydrogenase ([FeFe]‐H2ase) mimics, we report a new model approach for a photocatalytic [FeFe]‐H2ase mimic 1, which contains a 1‐silafluorene unit as a photosensitizer. Thereby, the photoactive ligand is linked to the [2Fe2S] cluster through S–CH2–Si bridges. Photochemical H2 evolution experiments were performed and revealed a turnover number (TON) of 29. This is the highest reported photocatalytic efficiency for an [FeFe]‐H2ase model complex in which the photosensitizer is covalently linked to the catalytic center.
We report a viable synthetic pathway for the construction of a new photoactive model of the [FeFe]‐hydrogenase ([FeFe]‐H2ase) active site with a dithiolate bridge and 1‐silafluorene as a photosensitizer. The [FeFe]‐H2ase mimic represents a very compact, easily accessible, and inexpensive photocatalyst for hydrogen generation. |
| doi_str_mv | 10.1002/ejic.201300537 |
| format | Article |
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We report a viable synthetic pathway for the construction of a new photoactive model of the [FeFe]‐hydrogenase ([FeFe]‐H2ase) active site with a dithiolate bridge and 1‐silafluorene as a photosensitizer. The [FeFe]‐H2ase mimic represents a very compact, easily accessible, and inexpensive photocatalyst for hydrogen generation.</description><identifier>ISSN: 1434-1948</identifier><identifier>EISSN: 1099-0682</identifier><identifier>DOI: 10.1002/ejic.201300537</identifier><language>eng</language><publisher>Weinheim: WILEY-VCH Verlag</publisher><subject>Accessibility ; Catalysis ; Catalysts ; Chemical Sciences ; Covalence ; Enzyme models ; Evolution ; Hydrogen ; Hydrogenase ; Iron ; Photocatalysis ; Photocatalysts ; Silicon ; Sulfur</subject><ispartof>European journal of inorganic chemistry, 2013-09, Vol.2013 (25), p.4466-4472</ispartof><rights>Copyright © 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>Distributed under a Creative Commons Attribution 4.0 International License</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c4887-8cec58cbb5f4544c64b5381e270454a6973848b672c31c13e0b7a246646461023</citedby><cites>FETCH-LOGICAL-c4887-8cec58cbb5f4544c64b5381e270454a6973848b672c31c13e0b7a246646461023</cites><orcidid>0000-0002-1777-8578 ; 0000-0001-8161-7878</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fejic.201300537$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fejic.201300537$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>230,314,780,784,885,1417,27924,27925,45574,45575</link.rule.ids><backlink>$$Uhttps://hal.univ-brest.fr/hal-01520727$$DView record in HAL$$Hfree_for_read</backlink></links><search><creatorcontrib>Goy, Roman</creatorcontrib><creatorcontrib>Apfel, Ulf-Peter</creatorcontrib><creatorcontrib>Elleouet, Catherine</creatorcontrib><creatorcontrib>Escudero, Daniel</creatorcontrib><creatorcontrib>Elstner, Martin</creatorcontrib><creatorcontrib>Görls, Helmar</creatorcontrib><creatorcontrib>Talarmin, Jean</creatorcontrib><creatorcontrib>Schollhammer, Philippe</creatorcontrib><creatorcontrib>González, Leticia</creatorcontrib><creatorcontrib>Weigand, Wolfgang</creatorcontrib><title>A Silicon-Heteroaromatic System as Photosensitizer for Light-Driven Hydrogen Production by Hydrogenase Mimics</title><title>European journal of inorganic chemistry</title><addtitle>Eur. J. Inorg. Chem</addtitle><description>The utilization of light and inexpensive catalysts to afford hydrogen represents a huge challenge. Following our interest in silicon‐containing [FeFe]‐hydrogenase ([FeFe]‐H2ase) mimics, we report a new model approach for a photocatalytic [FeFe]‐H2ase mimic 1, which contains a 1‐silafluorene unit as a photosensitizer. Thereby, the photoactive ligand is linked to the [2Fe2S] cluster through S–CH2–Si bridges. Photochemical H2 evolution experiments were performed and revealed a turnover number (TON) of 29. This is the highest reported photocatalytic efficiency for an [FeFe]‐H2ase model complex in which the photosensitizer is covalently linked to the catalytic center.
We report a viable synthetic pathway for the construction of a new photoactive model of the [FeFe]‐hydrogenase ([FeFe]‐H2ase) active site with a dithiolate bridge and 1‐silafluorene as a photosensitizer. The [FeFe]‐H2ase mimic represents a very compact, easily accessible, and inexpensive photocatalyst for hydrogen generation.</description><subject>Accessibility</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemical Sciences</subject><subject>Covalence</subject><subject>Enzyme models</subject><subject>Evolution</subject><subject>Hydrogen</subject><subject>Hydrogenase</subject><subject>Iron</subject><subject>Photocatalysis</subject><subject>Photocatalysts</subject><subject>Silicon</subject><subject>Sulfur</subject><issn>1434-1948</issn><issn>1099-0682</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2013</creationdate><recordtype>article</recordtype><recordid>eNqFkc1v1DAQxSNEJUrLlbMlLnDIMv5I7ByXtHRLl1JpQUhcLMed7XpJ4mJnC-Gvx6tUK8QF-eDx6PeenvWy7CWFGQVgb3Hr7IwB5QAFl0-yYwpVlUOp2NM0Cy5yWgn1LHse4xYAOPDyOOvmZOVaZ32fL3DA4E3wnRmcJasxDtgRE8nNxg8-Yh_d4H5jIGsfyNLdbYb8LLgH7MlivA3-Lg03wd_u7OB8T5rxsDYRyUfXORtPs6O1aSO-eLxPsi_vzz_Xi3z56eKyni9zK5SSubJoC2WbpliLQghbiqbgiiKTkN6mrCRXQjWlZJZTSzlCIw0TZSnSocD4SfZm8t2YVt8H15kwam-cXsyXer8DWjCQTD7QxL6e2Pvgf-wwDrpz0WLbmh79LmpagWBcqWpv--ofdOt3oU8_0ckvpZIpXqJmE2WDjzHg-pCAgt43pfdN6UNTSVBNgp-uxfE_tD7_cFn_rc0nrUtt_TpoTfiuy5Sn0F-vL7S8qlfX775xXfM_ySWlAA</recordid><startdate>20130902</startdate><enddate>20130902</enddate><creator>Goy, Roman</creator><creator>Apfel, Ulf-Peter</creator><creator>Elleouet, Catherine</creator><creator>Escudero, Daniel</creator><creator>Elstner, Martin</creator><creator>Görls, Helmar</creator><creator>Talarmin, Jean</creator><creator>Schollhammer, Philippe</creator><creator>González, Leticia</creator><creator>Weigand, Wolfgang</creator><general>WILEY-VCH Verlag</general><general>WILEY‐VCH Verlag</general><general>Wiley Subscription Services, Inc</general><general>Wiley-VCH Verlag</general><scope>BSCLL</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>1XC</scope><orcidid>https://orcid.org/0000-0002-1777-8578</orcidid><orcidid>https://orcid.org/0000-0001-8161-7878</orcidid></search><sort><creationdate>20130902</creationdate><title>A Silicon-Heteroaromatic System as Photosensitizer for Light-Driven Hydrogen Production by Hydrogenase Mimics</title><author>Goy, Roman ; Apfel, Ulf-Peter ; Elleouet, Catherine ; Escudero, Daniel ; Elstner, Martin ; Görls, Helmar ; Talarmin, Jean ; Schollhammer, Philippe ; González, Leticia ; Weigand, Wolfgang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c4887-8cec58cbb5f4544c64b5381e270454a6973848b672c31c13e0b7a246646461023</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2013</creationdate><topic>Accessibility</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Chemical Sciences</topic><topic>Covalence</topic><topic>Enzyme models</topic><topic>Evolution</topic><topic>Hydrogen</topic><topic>Hydrogenase</topic><topic>Iron</topic><topic>Photocatalysis</topic><topic>Photocatalysts</topic><topic>Silicon</topic><topic>Sulfur</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Goy, Roman</creatorcontrib><creatorcontrib>Apfel, Ulf-Peter</creatorcontrib><creatorcontrib>Elleouet, Catherine</creatorcontrib><creatorcontrib>Escudero, Daniel</creatorcontrib><creatorcontrib>Elstner, Martin</creatorcontrib><creatorcontrib>Görls, Helmar</creatorcontrib><creatorcontrib>Talarmin, Jean</creatorcontrib><creatorcontrib>Schollhammer, Philippe</creatorcontrib><creatorcontrib>González, Leticia</creatorcontrib><creatorcontrib>Weigand, Wolfgang</creatorcontrib><collection>Istex</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Hyper Article en Ligne (HAL)</collection><jtitle>European journal of inorganic chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Goy, Roman</au><au>Apfel, Ulf-Peter</au><au>Elleouet, Catherine</au><au>Escudero, Daniel</au><au>Elstner, Martin</au><au>Görls, Helmar</au><au>Talarmin, Jean</au><au>Schollhammer, Philippe</au><au>González, Leticia</au><au>Weigand, Wolfgang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>A Silicon-Heteroaromatic System as Photosensitizer for Light-Driven Hydrogen Production by Hydrogenase Mimics</atitle><jtitle>European journal of inorganic chemistry</jtitle><addtitle>Eur. J. Inorg. Chem</addtitle><date>2013-09-02</date><risdate>2013</risdate><volume>2013</volume><issue>25</issue><spage>4466</spage><epage>4472</epage><pages>4466-4472</pages><issn>1434-1948</issn><eissn>1099-0682</eissn><abstract>The utilization of light and inexpensive catalysts to afford hydrogen represents a huge challenge. Following our interest in silicon‐containing [FeFe]‐hydrogenase ([FeFe]‐H2ase) mimics, we report a new model approach for a photocatalytic [FeFe]‐H2ase mimic 1, which contains a 1‐silafluorene unit as a photosensitizer. Thereby, the photoactive ligand is linked to the [2Fe2S] cluster through S–CH2–Si bridges. Photochemical H2 evolution experiments were performed and revealed a turnover number (TON) of 29. This is the highest reported photocatalytic efficiency for an [FeFe]‐H2ase model complex in which the photosensitizer is covalently linked to the catalytic center.
We report a viable synthetic pathway for the construction of a new photoactive model of the [FeFe]‐hydrogenase ([FeFe]‐H2ase) active site with a dithiolate bridge and 1‐silafluorene as a photosensitizer. The [FeFe]‐H2ase mimic represents a very compact, easily accessible, and inexpensive photocatalyst for hydrogen generation.</abstract><cop>Weinheim</cop><pub>WILEY-VCH Verlag</pub><doi>10.1002/ejic.201300537</doi><tpages>7</tpages><orcidid>https://orcid.org/0000-0002-1777-8578</orcidid><orcidid>https://orcid.org/0000-0001-8161-7878</orcidid></addata></record> |
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| subjects | Accessibility Catalysis Catalysts Chemical Sciences Covalence Enzyme models Evolution Hydrogen Hydrogenase Iron Photocatalysis Photocatalysts Silicon Sulfur |
| title | A Silicon-Heteroaromatic System as Photosensitizer for Light-Driven Hydrogen Production by Hydrogenase Mimics |
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