Electron and proton transfers modulate DNA binding by the transcription regulator RsrR

Crack, Jason C., Amara, Patricia, Volbeda, Anne, Mouesca, Jean-Marie, Rohac, Roman, Pellicer Martinez, Maria, Huang, Chia-Ying, Gigarel, Océane, Rinaldi, Clara, Le Brun, Nick E. ORCID: https://orcid.org/0000-0001-9780-4061 and Fontecilla-Camps, Juan C. (2020) Electron and proton transfers modulate DNA binding by the transcription regulator RsrR. Journal of the American Chemical Society, 142 (11). pp. 5104-5116. ISSN 0002-7863

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The [Fe2S2]-RsrR gene transcription regulator senses the redox status in bacteria by modulating DNA binding, while its cluster cycles between +1 and +2 states-only the latter binds DNA. We have previously shown that RsrR can undergo remarkable conformational changes involving a 100° rotation of tryptophan 9 between exposed (Out) and buried (In) states. Here, we have used the chemical modification of Trp9, site-directed mutagenesis, and crystallographic and computational chemical studies to show that (i) the Out and In states correspond to oxidized and reduced RsrR, respectively, (ii) His33 is protonated in the In state due to a change in its pKa caused by cluster reduction, and (iii) Trp9 rotation is conditioned by the response of its dipole moment to environmental electrostatic changes. Our findings illustrate a novel function of protonation resulting from electron transfer.

Item Type: Article
Faculty \ School: Faculty of Science > School of Chemistry
UEA Research Groups: Faculty of Science > Research Groups > Chemistry of Life Processes
Faculty of Science > Research Centres > Centre for Molecular and Structural Biochemistry
Depositing User: LivePure Connector
Date Deposited: 19 Mar 2020 02:42
Last Modified: 22 Oct 2022 05:57
URI: https://ueaeprints.uea.ac.uk/id/eprint/74540
DOI: 10.1021/jacs.9b12250


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