Redox active iron nitrosyl units in proton reduction electrocatalysis

doi:10.1038/ncomms4684

淡江大學機構典藏 > 理學院 > 化學學系暨研究所 > 期刊論文 > Item 987654321/98607

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題名:	Redox active iron nitrosyl units in proton reduction electrocatalysis
作者:	Hsieh, Chung-Hung;Shengda Ding;Özlen F. Erdem;Danielle J. Crouthers;Tianbiao Liu;Charles C. L. McCrory;Wolfgang Lubitz;Codrina V. Popescu;Joseph H. Reibenspies;Michael B. Hall;Marcetta Y. Darensbourg
貢獻者:	淡江大學化學學系
關鍵詞:	Chemical sciences;Catalysis;Inorganic chemistry
日期:	2014-05-02
上傳時間:	2014-08-27 09:49:17 (UTC+8)
出版者:	London: Nature Publishing Group
摘要:	Base metal, molecular catalysts for the fundamental process of conversion of protons and electrons to dihydrogen, remain a substantial synthetic goal related to a sustainable energy future. Here we report a diiron complex with bridging thiolates in the butterfly shape of the 2Fe2S core of the [FeFe]-hydrogenase active site but with nitrosyl rather than carbonyl or cyanide ligands. This binuclear [(NO)Fe(N2S2)Fe(NO)2]+ complex maintains structural integrity in two redox levels; it consists of a (N2S2)Fe(NO) complex (N2S2=N,N′-bis(2-mercaptoethyl)-1,4-diazacycloheptane) that serves as redox active metallodithiolato bidentate ligand to a redox active dinitrosyl iron unit, Fe(NO)2. Experimental and theoretical methods demonstrate the accommodation of redox levels in both components of the complex, each involving electronically versatile nitrosyl ligands. An interplay of orbital mixing between the Fe(NO) and Fe(NO)2 sites and within the iron nitrosyl bonds in each moiety is revealed, accounting for the interactions that facilitate electron uptake, storage and proton reduction.
關聯:	Nature Communications 5, 3684
DOI:	10.1038/ncomms4684
顯示於類別:	[化學學系暨研究所] 期刊論文

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