Synthesis and Electrocatalytic Activity of [FeFe]‐Hydrogenase Model Complexes with Non‐Innocent Chelating Nitrogen‐Donor Ligands

Roy, Souvik; Laureanti, Joseph A.; Groy, Thomas L.; Jones, Anne K.

doi:10.1002/ejic.201700123

Title: Synthesis and Electrocatalytic Activity of [FeFe]‐Hydrogenase Model Complexes with Non‐Innocent Chelating Nitrogen‐Donor Ligands

Journal Article · Fri Apr 07 00:00:00 EDT 2017 · European Journal of Inorganic Chemistry

DOI:https://doi.org/10.1002/ejic.201700123· OSTI ID:1401057

^[1]; Laureanti, Joseph A. ^[1]; Groy, Thomas L. ^[1];

^[1]

School of Molecular Sciences Arizona State University 85287 Tempe Arizona USA

To probe the influence of redox non‐innocent ligands on a well‐known class of [FeFe]‐hydrogenase models, three new asymmetrically disubstituted diiron complexes of the general formula (µ‐SRS)[Fe(CO) ₃ ][Fe(CO)(N‐N)] {SRS = propane‐1,3‐dithiolate (pdt) or benzene‐1,2‐dithiolate (bdt), and N‐N = 2,2′‐bipyridine (bipy) or 2,2′‐bipyrimidine (bpym)} have been synthesized from their parent hexacarbonyls and characterized. The new complexes, (µ‐pdt)Fe ₂ (CO) ₄ (κ ² ‐bpym) ( 2 ), (µ‐bdt)Fe ₂ (CO) ₄ (κ ² ‐bipy) ( 3 ), and (µ‐bdt)Fe ₂ (CO) ₄ (κ ² ‐bpym) ( 4 ), were fully characterized by spectroscopic and electrochemical techniques, and the results are compared to those of a related complex, (µ‐pdt)Fe ₂ (CO) ₄ (κ ² ‐bipy) ( 1 ). The crystal structures of 2 – 4 show that, in each complex, the two iron units are in an eclipsed orientation, and the N‐N ligand lies in the basal plane. IR spectra and electrochemical analyses indicate that electron density at the iron centers decreases in the order 1 > 2 > 3 > 4 . Furthermore, compound 2 undergoes a ligand‐centered reduction at the same potential that the hexacarbonyl precursor undergoes its first reduction. However, unlike the 2,2′‐bipy derivatives 1 and 3 , the 2,2′‐bpym complexes 2 and 4 are not effective catalysts for electrochemical proton reduction from acetic acid.

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Sponsoring Organization:: USDOE

OSTI ID:: 1401057

Journal Information:: European Journal of Inorganic Chemistry, Journal Name: European Journal of Inorganic Chemistry Vol. 2017 Journal Issue: 23; ISSN 1434-1948

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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