ADT-Type [FeFe]-hydrogenase biomimics featuring monodentate phosphines: formation, structures, and electrocatalysis

To further develop the diiron subsite biomimics of [FeFe]-hydrogenases, two new diiron azadithiolate (adt) complexes Fe 2 ( μ -adt NPh )(CO) 5 (Ph 2 PX) (X = NHBu t , 1 and P(O)Ph 2 , 2 ) featuring monodentate phosphines were unexpectedly produced by the Me 3 NO-induced decarbonylating reactions of...

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Veröffentlicht in:Transition metal chemistry (Weinheim) 2021-12, Vol.46 (8), p.645-653
Hauptverfasser: Chen, Fei-Yan, Hu, Meng-Yuan, Gu, Xiao-Li, Liu, Xu-Feng, Zhao, Pei-Hua
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creator Chen, Fei-Yan
Hu, Meng-Yuan
Gu, Xiao-Li
Liu, Xu-Feng
Zhao, Pei-Hua
description To further develop the diiron subsite biomimics of [FeFe]-hydrogenases, two new diiron azadithiolate (adt) complexes Fe 2 ( μ -adt NPh )(CO) 5 (Ph 2 PX) (X = NHBu t , 1 and P(O)Ph 2 , 2 ) featuring monodentate phosphines were unexpectedly produced by the Me 3 NO-induced decarbonylating reactions of all-CO diiron precursor Fe 2 ( μ -adt NPh )(CO) 6 ( A , adt NPh  = (SCH 2 ) 2 NPh) with different aminodiphosphines (Ph 2 P) 2 NR (R = Bu t and C 6 H 4 Cl- p ) in MeCN at ambient temperature. The as-obtained complexes 1 and 2 have been fully characterized by means of elemental analysis, FT-IR, ( 1 H, 31 P) NMR spectroscopies and further confirmed by X-ray crystallography. At the same time, the electrochemical and electrocatalytic behaviors of 1 and 2 have been studied and compared in the absence or presence of acetic acid (HOAc) as a proton source by cyclic voltammetry (CV), suggesting that they can be considered as the active biomimetic electrocatalysts for proton reduction to hydrogen (H 2 ).
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At the same time, the electrochemical and electrocatalytic behaviors of 1 and 2 have been studied and compared in the absence or presence of acetic acid (HOAc) as a proton source by cyclic voltammetry (CV), suggesting that they can be considered as the active biomimetic electrocatalysts for proton reduction to hydrogen (H 2 ).</description><identifier>ISSN: 0340-4285</identifier><identifier>EISSN: 1572-901X</identifier><identifier>DOI: 10.1007/s11243-021-00482-4</identifier><language>eng</language><publisher>Cham: Springer International Publishing</publisher><subject>Acetic acid ; Ambient temperature ; Biomimetics ; Carbon monoxide ; Catalysis ; Chemical analysis ; Chemistry ; Chemistry and Materials Science ; Crystallography ; Electrocatalysts ; Hydrogenase ; Infrared analysis ; Inorganic Chemistry ; NMR ; Nuclear magnetic resonance ; Organometallic Chemistry ; Phosphines ; Physical Chemistry ; Protons</subject><ispartof>Transition metal chemistry (Weinheim), 2021-12, Vol.46 (8), p.645-653</ispartof><rights>The Author(s), under exclusive licence to Springer Nature Switzerland AG 2021</rights><rights>The Author(s), under exclusive licence to Springer Nature Switzerland AG 2021.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c319t-76f045066ee6fa602503b5bc7b18923d3e6dad63a55ce2c6eb09629bbf94854c3</citedby><cites>FETCH-LOGICAL-c319t-76f045066ee6fa602503b5bc7b18923d3e6dad63a55ce2c6eb09629bbf94854c3</cites><orcidid>0000-0002-5480-6128</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1007/s11243-021-00482-4$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s11243-021-00482-4$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>314,776,780,27903,27904,41467,42536,51297</link.rule.ids></links><search><creatorcontrib>Chen, Fei-Yan</creatorcontrib><creatorcontrib>Hu, Meng-Yuan</creatorcontrib><creatorcontrib>Gu, Xiao-Li</creatorcontrib><creatorcontrib>Liu, Xu-Feng</creatorcontrib><creatorcontrib>Zhao, Pei-Hua</creatorcontrib><title>ADT-Type [FeFe]-hydrogenase biomimics featuring monodentate phosphines: formation, structures, and electrocatalysis</title><title>Transition metal chemistry (Weinheim)</title><addtitle>Transit Met Chem</addtitle><description>To further develop the diiron subsite biomimics of [FeFe]-hydrogenases, two new diiron azadithiolate (adt) complexes Fe 2 ( μ -adt NPh )(CO) 5 (Ph 2 PX) (X = NHBu t , 1 and P(O)Ph 2 , 2 ) featuring monodentate phosphines were unexpectedly produced by the Me 3 NO-induced decarbonylating reactions of all-CO diiron precursor Fe 2 ( μ -adt NPh )(CO) 6 ( A , adt NPh  = (SCH 2 ) 2 NPh) with different aminodiphosphines (Ph 2 P) 2 NR (R = Bu t and C 6 H 4 Cl- p ) in MeCN at ambient temperature. 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At the same time, the electrochemical and electrocatalytic behaviors of 1 and 2 have been studied and compared in the absence or presence of acetic acid (HOAc) as a proton source by cyclic voltammetry (CV), suggesting that they can be considered as the active biomimetic electrocatalysts for proton reduction to hydrogen (H 2 ).</description><subject>Acetic acid</subject><subject>Ambient temperature</subject><subject>Biomimetics</subject><subject>Carbon monoxide</subject><subject>Catalysis</subject><subject>Chemical analysis</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Crystallography</subject><subject>Electrocatalysts</subject><subject>Hydrogenase</subject><subject>Infrared analysis</subject><subject>Inorganic Chemistry</subject><subject>NMR</subject><subject>Nuclear magnetic resonance</subject><subject>Organometallic Chemistry</subject><subject>Phosphines</subject><subject>Physical Chemistry</subject><subject>Protons</subject><issn>0340-4285</issn><issn>1572-901X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp9kE9rGzEQR0VooG6SL5CTINcoHf1db28hidNCoBcXCqUIrXbWXuNdbTXywd8-m7qQW09zeb838Bi7lnAnAarPJKUyWoCSAsAslTBnbCFtpUQN8ucHtgBtQBi1tB_ZJ6IdAFhVmQWj-8e1WB8n5L9WuMLfYntsc9rgGAh506ehH_pIvMNQDrkfN3xIY2pxLKEgn7aJpm0_In3hXcpDKH0abzmVfIgzjnTLw9hy3GMsOcVQwv5IPV2y8y7sCa_-3Qv2Y_W0fvgqXr4_f3u4fxFRy7qIynVgLDiH6LrgQFnQjW1i1chlrXSr0bWhdTpYG1FFhw3UTtVN09VmaU3UF-zm5J1y-nNAKn6XDnmcX3o160BrK91MqRMVcyLK2Pkp90PIRy_Bv8X1p7h-juv_xvVmHunTiKa3Kpjf1f9ZvQIygH6r</recordid><startdate>20211201</startdate><enddate>20211201</enddate><creator>Chen, Fei-Yan</creator><creator>Hu, Meng-Yuan</creator><creator>Gu, Xiao-Li</creator><creator>Liu, Xu-Feng</creator><creator>Zhao, Pei-Hua</creator><general>Springer International Publishing</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><orcidid>https://orcid.org/0000-0002-5480-6128</orcidid></search><sort><creationdate>20211201</creationdate><title>ADT-Type [FeFe]-hydrogenase biomimics featuring monodentate phosphines: formation, structures, and electrocatalysis</title><author>Chen, Fei-Yan ; Hu, Meng-Yuan ; Gu, Xiao-Li ; Liu, Xu-Feng ; Zhao, Pei-Hua</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c319t-76f045066ee6fa602503b5bc7b18923d3e6dad63a55ce2c6eb09629bbf94854c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Acetic acid</topic><topic>Ambient temperature</topic><topic>Biomimetics</topic><topic>Carbon monoxide</topic><topic>Catalysis</topic><topic>Chemical analysis</topic><topic>Chemistry</topic><topic>Chemistry and Materials Science</topic><topic>Crystallography</topic><topic>Electrocatalysts</topic><topic>Hydrogenase</topic><topic>Infrared analysis</topic><topic>Inorganic Chemistry</topic><topic>NMR</topic><topic>Nuclear magnetic resonance</topic><topic>Organometallic Chemistry</topic><topic>Phosphines</topic><topic>Physical Chemistry</topic><topic>Protons</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chen, Fei-Yan</creatorcontrib><creatorcontrib>Hu, Meng-Yuan</creatorcontrib><creatorcontrib>Gu, Xiao-Li</creatorcontrib><creatorcontrib>Liu, Xu-Feng</creatorcontrib><creatorcontrib>Zhao, Pei-Hua</creatorcontrib><collection>CrossRef</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><jtitle>Transition metal chemistry (Weinheim)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chen, Fei-Yan</au><au>Hu, Meng-Yuan</au><au>Gu, Xiao-Li</au><au>Liu, Xu-Feng</au><au>Zhao, Pei-Hua</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>ADT-Type [FeFe]-hydrogenase biomimics featuring monodentate phosphines: formation, structures, and electrocatalysis</atitle><jtitle>Transition metal chemistry (Weinheim)</jtitle><stitle>Transit Met Chem</stitle><date>2021-12-01</date><risdate>2021</risdate><volume>46</volume><issue>8</issue><spage>645</spage><epage>653</epage><pages>645-653</pages><issn>0340-4285</issn><eissn>1572-901X</eissn><abstract>To further develop the diiron subsite biomimics of [FeFe]-hydrogenases, two new diiron azadithiolate (adt) complexes Fe 2 ( μ -adt NPh )(CO) 5 (Ph 2 PX) (X = NHBu t , 1 and P(O)Ph 2 , 2 ) featuring monodentate phosphines were unexpectedly produced by the Me 3 NO-induced decarbonylating reactions of all-CO diiron precursor Fe 2 ( μ -adt NPh )(CO) 6 ( A , adt NPh  = (SCH 2 ) 2 NPh) with different aminodiphosphines (Ph 2 P) 2 NR (R = Bu t and C 6 H 4 Cl- p ) in MeCN at ambient temperature. 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subjects Acetic acid
Ambient temperature
Biomimetics
Carbon monoxide
Catalysis
Chemical analysis
Chemistry
Chemistry and Materials Science
Crystallography
Electrocatalysts
Hydrogenase
Infrared analysis
Inorganic Chemistry
NMR
Nuclear magnetic resonance
Organometallic Chemistry
Phosphines
Physical Chemistry
Protons
title ADT-Type [FeFe]-hydrogenase biomimics featuring monodentate phosphines: formation, structures, and electrocatalysis
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