Spectroscopic and electrochemical investigation of electrocatalytic proton reduction by Fe2(μ-pdt)(CO)6, 1, have been interpreted in terms of a reaction scheme involving sequential electron–proton reactions to give a two-electron, two-proton product that undergoes rate-limiting dihydrogen elimination. Further reduction, at slightly higher negative potentials, gives a more reactive product and this process dominates reactions conducted at higher acid concentrations. Inhibition of the electrocatalytic reaction by CO is due to the more efficient loss of catalyst and this is best modelled by a reaction that is second order in terms of 1−. During electrocatalytic proton reduction a new species is observed, which features a bridging CO group and the wavenumbers of the ν(CO) modes of the terminally bound carbonyl groups are similar to those of the carbonyl groups bound to the oxidized form of the H-cluster.
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Conference Article|
February 01 2005
Electrocatalytic proton reduction by dithiolate-bridged diiron carbonyl complexes: a connection to the H-cluster?
S.J. Borg;
S.J. Borg
*School of Chemistry, University of Melbourne, Victoria 3010, Australia
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M.I. Bondin;
M.I. Bondin
*School of Chemistry, University of Melbourne, Victoria 3010, Australia
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S.P. Best;
S.P. Best
1
*School of Chemistry, University of Melbourne, Victoria 3010, Australia
1Correspondence may be addressed to either of the authors (email spbest@unimelb.edu.au and chris.pickett@bbsrc.ac.uk).
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M. Razavet;
M. Razavet
†Department of Biological Chemistry, John Innes Centre, Norwich Research Park, Colney, Norwich NR4 7UH, U.K.
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X. Liu;
X. Liu
†Department of Biological Chemistry, John Innes Centre, Norwich Research Park, Colney, Norwich NR4 7UH, U.K.
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C.J. Pickett
C.J. Pickett
1
†Department of Biological Chemistry, John Innes Centre, Norwich Research Park, Colney, Norwich NR4 7UH, U.K.
1Correspondence may be addressed to either of the authors (email spbest@unimelb.edu.au and chris.pickett@bbsrc.ac.uk).
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Publisher: Portland Press Ltd
Received:
September 30 2004
Online ISSN: 1470-8752
Print ISSN: 0300-5127
© 2005 The Biochemical Society
2005
Biochem Soc Trans (2005) 33 (1): 3–6.
Article history
Received:
September 30 2004
Citation
S.J. Borg, M.I. Bondin, S.P. Best, M. Razavet, X. Liu, C.J. Pickett; Electrocatalytic proton reduction by dithiolate-bridged diiron carbonyl complexes: a connection to the H-cluster?. Biochem Soc Trans 1 February 2005; 33 (1): 3–6. doi: https://doi.org/10.1042/BST0330003
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