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Serrano, Pauline N., Wang, Hongxin, Crack, Jason C., Prior, Christopher, Hutchings, Matthew I., Thomson, Andrew J., Kamali, Saeed, Yoda, Yoshitaka, Zhao, Jiyong, Hu, Michael Y., Alp, Ercan E., Oganesyan, Vasily S. 
ORCID: https://orcid.org/0000-0002-8738-1146, Le Brun, Nick E. ORCID: https://orcid.org/0000-0001-9780-4061 and Cramer, Stephen P.
(2016)
Nitrosylation of nitric-oxide-sensing regulatory proteins containing [4Fe-4S] clusters gives rise to multiple iron-nitrosyl complexes.
Angewandte Chemie International Edition, 55 (47).
14575–14579.
ISSN 1433-7851
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Abstract
The reaction of protein-bound iron–sulfur (Fe-S) clusters with nitric oxide (NO) plays key roles in NO-mediated toxicity and signaling. Elucidation of the mechanism of the reaction of NO with DNA regulatory proteins that contain Fe-S clusters has been hampered by a lack of information about the nature of the iron-nitrosyl products formed. Herein, we report nuclear resonance vibrational spectroscopy (NRVS) and density functional theory (DFT) calculations that identify NO reaction products in WhiD and NsrR, regulatory proteins that use a [4Fe-4S] cluster to sense NO. This work reveals that nitrosylation yields multiple products structurally related to Roussin's Red Ester (RRE, [Fe2(NO)4(Cys)2]) and Roussin's Black Salt (RBS, [Fe4(NO)7S3]. In the latter case, the absence of 32S/34S shifts in the Fe−S region of the NRVS spectra suggest that a new species, Roussin's Black Ester (RBE), may be formed, in which one or more of the sulfide ligands is replaced by Cys thiolates.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | gene regulation,iron–sulfur clusters,nitric oxide,nuclear vibrational resonance spectroscopy,synchrotron radiation |
| Faculty \ School: | Faculty of Science > School of Chemistry Faculty of Science Faculty of Science > School of Biological Sciences |
| UEA Research Groups: | Faculty of Science > Research Groups > Molecular Microbiology Faculty of Science > Research Groups > Biophysical Chemistry (former - to 2017) Faculty of Science > Research Centres > Centre for Molecular and Structural Biochemistry Faculty of Science > Research Groups > Organisms and the Environment Faculty of Science > Research Groups > Chemistry of Light and Energy Faculty of Science > Research Groups > Chemistry of Life Processes Faculty of Science > Research Groups > Centre for Photonics and Quantum Science |
| Depositing User: | Pure Connector |
| Date Deposited: | 11 Oct 2016 16:00 |
| Last Modified: | 11 May 2023 20:31 |
| URI: | https://ueaeprints.uea.ac.uk/id/eprint/60858 |
| DOI: | 10.1002/anie.201607033 |
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