Electronic and geometric effects of phosphatriazaadamantane ligands on the catalytic activity of an [FeFe] hydrogenase inspired complex
The [FeFe] hydrogenase enzyme active site inspired complexes [Fe(2)(mu-C(6)H(4)S(2))(CO)(5)PTA] (1PTA) and [Fe(2)(mu-C(6)H(4)S(2))(CO)(4)PTA(2)] (1PTA(2)) (PTA = 1,3,5-triaza-7-phosphaadamantane) were synthesized and characterized. The ability of 1PTA and 1PTA(2) to catalytically produce molecular h...
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| Veröffentlicht in: | Dalton transactions : an international journal of inorganic chemistry 2010-01, Vol.39 (12), p.3050-3056 |
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| container_title | Dalton transactions : an international journal of inorganic chemistry |
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| creator | Vannucci, Aaron K Wang, Shihua Nichol, Gary S Lichtenberger, Dennis L Evans, Dennis H Glass, Richard S |
| description | The [FeFe] hydrogenase enzyme active site inspired complexes [Fe(2)(mu-C(6)H(4)S(2))(CO)(5)PTA] (1PTA) and [Fe(2)(mu-C(6)H(4)S(2))(CO)(4)PTA(2)] (1PTA(2)) (PTA = 1,3,5-triaza-7-phosphaadamantane) were synthesized and characterized. The ability of 1PTA and 1PTA(2) to catalytically produce molecular hydrogen in solution from the weak acid acetic acid was examined electrochemically and compared to previous studies on the all carbonyl containing analogue [Fe(2)(mu-C(6)H(4)S(2))(CO)(6)] (1). Computational methods and cyclic voltammograms indicated that the substitution of CO ligands by PTA in 1 resulted in markedly different reduction chemistry. Both 1PTA and 1PTA(2) catalytically produce molecular hydrogen from acetic acid, however, the mechanism by which and 1PTA and 1PTA(2) catalyze hydrogen differ in the initial reductive processes. |
| doi_str_mv | 10.1039/b921067a |
| format | Article |
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The ability of 1PTA and 1PTA(2) to catalytically produce molecular hydrogen in solution from the weak acid acetic acid was examined electrochemically and compared to previous studies on the all carbonyl containing analogue [Fe(2)(mu-C(6)H(4)S(2))(CO)(6)] (1). Computational methods and cyclic voltammograms indicated that the substitution of CO ligands by PTA in 1 resulted in markedly different reduction chemistry. Both 1PTA and 1PTA(2) catalytically produce molecular hydrogen from acetic acid, however, the mechanism by which and 1PTA and 1PTA(2) catalyze hydrogen differ in the initial reductive processes.</description><identifier>ISSN: 1477-9226</identifier><identifier>EISSN: 1477-9234</identifier><identifier>DOI: 10.1039/b921067a</identifier><identifier>PMID: 20221539</identifier><language>eng</language><publisher>England</publisher><subject>Acetic acid ; Adamantane - analogs & derivatives ; Adamantane - chemistry ; Analogue ; Carbon monoxide ; Catalysis ; Crystallography, X-Ray ; Electrochemistry ; Electronics ; Enzymes ; Hydrogenase ; Hydrogenase - chemistry ; Hydrogenase - metabolism ; Iron-Sulfur Proteins - chemistry ; Iron-Sulfur Proteins - metabolism ; Ligands ; Models, Molecular ; Molecular Structure ; Organophosphorus Compounds - chemistry ; Oxidation-Reduction</subject><ispartof>Dalton transactions : an international journal of inorganic chemistry, 2010-01, Vol.39 (12), p.3050-3056</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c414t-949c3f0359b05ce90ff51a21c47186dc476eedb7f528c12122d3443b6d7be7613</citedby><cites>FETCH-LOGICAL-c414t-949c3f0359b05ce90ff51a21c47186dc476eedb7f528c12122d3443b6d7be7613</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/20221539$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Vannucci, Aaron K</creatorcontrib><creatorcontrib>Wang, Shihua</creatorcontrib><creatorcontrib>Nichol, Gary S</creatorcontrib><creatorcontrib>Lichtenberger, Dennis L</creatorcontrib><creatorcontrib>Evans, Dennis H</creatorcontrib><creatorcontrib>Glass, Richard S</creatorcontrib><title>Electronic and geometric effects of phosphatriazaadamantane ligands on the catalytic activity of an [FeFe] hydrogenase inspired complex</title><title>Dalton transactions : an international journal of inorganic chemistry</title><addtitle>Dalton Trans</addtitle><description>The [FeFe] hydrogenase enzyme active site inspired complexes [Fe(2)(mu-C(6)H(4)S(2))(CO)(5)PTA] (1PTA) and [Fe(2)(mu-C(6)H(4)S(2))(CO)(4)PTA(2)] (1PTA(2)) (PTA = 1,3,5-triaza-7-phosphaadamantane) were synthesized and characterized. The ability of 1PTA and 1PTA(2) to catalytically produce molecular hydrogen in solution from the weak acid acetic acid was examined electrochemically and compared to previous studies on the all carbonyl containing analogue [Fe(2)(mu-C(6)H(4)S(2))(CO)(6)] (1). Computational methods and cyclic voltammograms indicated that the substitution of CO ligands by PTA in 1 resulted in markedly different reduction chemistry. Both 1PTA and 1PTA(2) catalytically produce molecular hydrogen from acetic acid, however, the mechanism by which and 1PTA and 1PTA(2) catalyze hydrogen differ in the initial reductive processes.</description><subject>Acetic acid</subject><subject>Adamantane - analogs & derivatives</subject><subject>Adamantane - chemistry</subject><subject>Analogue</subject><subject>Carbon monoxide</subject><subject>Catalysis</subject><subject>Crystallography, X-Ray</subject><subject>Electrochemistry</subject><subject>Electronics</subject><subject>Enzymes</subject><subject>Hydrogenase</subject><subject>Hydrogenase - chemistry</subject><subject>Hydrogenase - metabolism</subject><subject>Iron-Sulfur Proteins - chemistry</subject><subject>Iron-Sulfur Proteins - metabolism</subject><subject>Ligands</subject><subject>Models, Molecular</subject><subject>Molecular Structure</subject><subject>Organophosphorus Compounds - chemistry</subject><subject>Oxidation-Reduction</subject><issn>1477-9226</issn><issn>1477-9234</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2010</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqN0c1qGzEQB3AREhrXKeQJim7Jxa0-V9YxNXZbMPSSnEIwWmlkb9hdbSU5xH2BvHZk7KS30tOMpN_8QQxCl5R8oYTrr7VmlFTKnKARFUpNNOPi9L1n1Tn6mNIjIYwRyT6gc1Y6KrkeoZd5CzbH0DcWm97hNYQOciwn8L68JBw8HjYhDRtTrs0fY5zpTJ9ND7ht1mWmkB7nDWBrsml3eZ9kc_PU5N1-2PT4fgELeMCbnYthDb1JgJs-DU0Eh23ohhaeL9CZN22CT8c6RneL-e3sx2T56_vP2c1yYgUVeaKFttwTLnVNpAVNvJfUMGqFotPKlVIBuFp5yaaWMsqY40LwunKqBlVRPkZXh9whht9bSHnVNclC25b_hG1aKc4ll1JVRV7_U1LFCdFSVv9BCZ-yqaCS_qU2hpQi-NUQm87EXUF7p1ffDru8KfTzMXVbd-De4dvy-CspUZov</recordid><startdate>20100101</startdate><enddate>20100101</enddate><creator>Vannucci, Aaron K</creator><creator>Wang, Shihua</creator><creator>Nichol, Gary S</creator><creator>Lichtenberger, Dennis L</creator><creator>Evans, Dennis H</creator><creator>Glass, Richard S</creator><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SP</scope><scope>7U5</scope><scope>8FD</scope><scope>L7M</scope><scope>7SR</scope><scope>8BQ</scope><scope>JG9</scope><scope>7X8</scope></search><sort><creationdate>20100101</creationdate><title>Electronic and geometric effects of phosphatriazaadamantane ligands on the catalytic activity of an [FeFe] hydrogenase inspired complex</title><author>Vannucci, Aaron K ; Wang, Shihua ; Nichol, Gary S ; Lichtenberger, Dennis L ; Evans, Dennis H ; Glass, Richard S</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c414t-949c3f0359b05ce90ff51a21c47186dc476eedb7f528c12122d3443b6d7be7613</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2010</creationdate><topic>Acetic acid</topic><topic>Adamantane - analogs & derivatives</topic><topic>Adamantane - chemistry</topic><topic>Analogue</topic><topic>Carbon monoxide</topic><topic>Catalysis</topic><topic>Crystallography, X-Ray</topic><topic>Electrochemistry</topic><topic>Electronics</topic><topic>Enzymes</topic><topic>Hydrogenase</topic><topic>Hydrogenase - chemistry</topic><topic>Hydrogenase - metabolism</topic><topic>Iron-Sulfur Proteins - chemistry</topic><topic>Iron-Sulfur Proteins - metabolism</topic><topic>Ligands</topic><topic>Models, Molecular</topic><topic>Molecular Structure</topic><topic>Organophosphorus Compounds - chemistry</topic><topic>Oxidation-Reduction</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Vannucci, Aaron K</creatorcontrib><creatorcontrib>Wang, Shihua</creatorcontrib><creatorcontrib>Nichol, Gary S</creatorcontrib><creatorcontrib>Lichtenberger, Dennis L</creatorcontrib><creatorcontrib>Evans, Dennis H</creatorcontrib><creatorcontrib>Glass, Richard S</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Electronics & Communications Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>Technology Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Materials Research Database</collection><collection>MEDLINE - Academic</collection><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Vannucci, Aaron K</au><au>Wang, Shihua</au><au>Nichol, Gary S</au><au>Lichtenberger, Dennis L</au><au>Evans, Dennis H</au><au>Glass, Richard S</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Electronic and geometric effects of phosphatriazaadamantane ligands on the catalytic activity of an [FeFe] hydrogenase inspired complex</atitle><jtitle>Dalton transactions : an international journal of inorganic chemistry</jtitle><addtitle>Dalton Trans</addtitle><date>2010-01-01</date><risdate>2010</risdate><volume>39</volume><issue>12</issue><spage>3050</spage><epage>3056</epage><pages>3050-3056</pages><issn>1477-9226</issn><eissn>1477-9234</eissn><abstract>The [FeFe] hydrogenase enzyme active site inspired complexes [Fe(2)(mu-C(6)H(4)S(2))(CO)(5)PTA] (1PTA) and [Fe(2)(mu-C(6)H(4)S(2))(CO)(4)PTA(2)] (1PTA(2)) (PTA = 1,3,5-triaza-7-phosphaadamantane) were synthesized and characterized. The ability of 1PTA and 1PTA(2) to catalytically produce molecular hydrogen in solution from the weak acid acetic acid was examined electrochemically and compared to previous studies on the all carbonyl containing analogue [Fe(2)(mu-C(6)H(4)S(2))(CO)(6)] (1). Computational methods and cyclic voltammograms indicated that the substitution of CO ligands by PTA in 1 resulted in markedly different reduction chemistry. Both 1PTA and 1PTA(2) catalytically produce molecular hydrogen from acetic acid, however, the mechanism by which and 1PTA and 1PTA(2) catalyze hydrogen differ in the initial reductive processes.</abstract><cop>England</cop><pmid>20221539</pmid><doi>10.1039/b921067a</doi><tpages>7</tpages></addata></record> |
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| source | MEDLINE; Royal Society Of Chemistry Journals 2008-; Alma/SFX Local Collection |
| subjects | Acetic acid Adamantane - analogs & derivatives Adamantane - chemistry Analogue Carbon monoxide Catalysis Crystallography, X-Ray Electrochemistry Electronics Enzymes Hydrogenase Hydrogenase - chemistry Hydrogenase - metabolism Iron-Sulfur Proteins - chemistry Iron-Sulfur Proteins - metabolism Ligands Models, Molecular Molecular Structure Organophosphorus Compounds - chemistry Oxidation-Reduction |
| title | Electronic and geometric effects of phosphatriazaadamantane ligands on the catalytic activity of an [FeFe] hydrogenase inspired complex |
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