Catalytic Hydrogen Evolution from Mononuclear Iron(II) Carbonyl Complexes as Minimal Functional Models of the [FeFe] Hydrogenase Active Site | Zendy

KaurGhumaan Sandeep | Zendy; Schwartz Lennart | Zendy; Lomoth Reiner | Zendy; Stein Matthias | Zendy; Ott Sascha | Zendy

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Catalytic Hydrogen Evolution from Mononuclear Iron(II) Carbonyl Complexes as Minimal Functional Models of the [FeFe] Hydrogenase Active Site

Author(s) -

KaurGhumaan Sandeep,

Schwartz Lennart,

Lomoth Reiner,

Stein Matthias,

Ott Sascha

Publication year - 2010

Publication title -

angewandte chemie international edition

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 5.831

H-Index - 550

eISSN - 1521-3773

pISSN - 1433-7851

DOI - 10.1002/anie.201002719

Subject(s) - hydrogenase , chemistry , catalysis , active site , protonation , hydrogen , electrochemistry , bond cleavage , density functional theory , photochemistry , cleavage (geology) , combinatorial chemistry , computational chemistry , organic chemistry , materials science , ion , electrode , fracture (geology) , composite material

How much iron does it take? Mononuclear complexes [Fe II (3,6‐R 2 bdt)(CO) 2 (PMe 3 ) 2 ] (bdt=1,2‐C 6 H 4 (S − ) 2 ; R=H, Cl) can be reversibly protonated at the sulfur ligands, can catalyze the electrochemical reduction of protons, and are thus minimal functional models of the [FeFe] hydrogenases (see scheme). DFT calculations show that cleavage of an FeS bond leads to the generation of a free coordination site, which is crucial for the formation of hydrides that are key intermediates in the generation of hydrogen.

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