Synthesis and Electrocatalytic Activity of [FeFe]‐Hydrogenase Model Complexes with Non‐Innocent Chelating Nitrogen‐Donor Ligands
Abstract
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′‐bpymmore »
- Authors:
-
- School of Molecular Sciences Arizona State University 85287 Tempe Arizona USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1401057
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- European Journal of Inorganic Chemistry
- Additional Journal Information:
- Journal Name: European Journal of Inorganic Chemistry Journal Volume: 2017 Journal Issue: 23; Journal ID: ISSN 1434-1948
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Roy, Souvik, Laureanti, Joseph A., Groy, Thomas L., and Jones, Anne K. Synthesis and Electrocatalytic Activity of [FeFe]‐Hydrogenase Model Complexes with Non‐Innocent Chelating Nitrogen‐Donor Ligands. Germany: N. p., 2017.
Web. doi:10.1002/ejic.201700123.
Roy, Souvik, Laureanti, Joseph A., Groy, Thomas L., & Jones, Anne K. Synthesis and Electrocatalytic Activity of [FeFe]‐Hydrogenase Model Complexes with Non‐Innocent Chelating Nitrogen‐Donor Ligands. Germany. https://doi.org/10.1002/ejic.201700123
Roy, Souvik, Laureanti, Joseph A., Groy, Thomas L., and Jones, Anne K. Fri .
"Synthesis and Electrocatalytic Activity of [FeFe]‐Hydrogenase Model Complexes with Non‐Innocent Chelating Nitrogen‐Donor Ligands". Germany. https://doi.org/10.1002/ejic.201700123.
@article{osti_1401057,
title = {Synthesis and Electrocatalytic Activity of [FeFe]‐Hydrogenase Model Complexes with Non‐Innocent Chelating Nitrogen‐Donor Ligands},
author = {Roy, Souvik and Laureanti, Joseph A. and Groy, Thomas L. and Jones, Anne K.},
abstractNote = {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.},
doi = {10.1002/ejic.201700123},
journal = {European Journal of Inorganic Chemistry},
number = 23,
volume = 2017,
place = {Germany},
year = {Fri Apr 07 00:00:00 EDT 2017},
month = {Fri Apr 07 00:00:00 EDT 2017}
}
https://doi.org/10.1002/ejic.201700123
Web of Science
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