Redox active iron nitrosyl units in proton reduction electrocatalysis
學年 102
學期 2
出版（發表）日期 2014-05-02
作品名稱 Redox active iron nitrosyl units in proton reduction electrocatalysis
作品名稱（其他語言）
著者 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
單位 淡江大學化學學系
出版者 London: Nature Publishing Group
著錄名稱、卷期、頁數 Nature Communications 5, 3684
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.
關鍵字 Chemical sciences;Catalysis;Inorganic chemistry
語言 en
ISSN 2041-1723
期刊性質 國外
收錄於 SCI
產學合作
通訊作者 Marcetta Y. Darensbourg
審稿制度 是
國別 GBR
公開徵稿
出版型式 ,電子版
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