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Issue 4, 2018
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A charge polarization model for the metal-specific activity of superoxide dismutases

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Abstract

The pathogenicity of Staphylococcus aureus is enhanced by having two superoxide dismutases (SODs): a Mn-specific SOD and another that can use either Mn or Fe. Using 94 GHz electron-nuclear double resonance (ENDOR) and electron double resonance detected (ELDOR)-NMR we show that, despite their different metal-specificities, their structural and electronic similarities extend down to their active-site 1H– and 14N–Mn(II) hyperfine interactions. However these interactions, and hence the positions of these nuclei, are different in the inactive Mn-reconstituted Escherichia coli Fe-specific SOD. Density functional theory modelling attributes this to a different angular position of the E. coli H171 ligand. This likely disrupts the Mn–H171–E170′ triad causing a shift in charge and in metal redox potential, leading to the loss of activity. This is supported by the correlated differences in the Mn(II) zero-field interactions of the three SOD types and suggests that the triad is important for determining metal specific activity.

Graphical abstract: A charge polarization model for the metal-specific activity of superoxide dismutases

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Publication details

The article was received on 06 Oct 2017, accepted on 18 Dec 2017 and first published on 18 Dec 2017


Article type: Paper
DOI: 10.1039/C7CP06829H
Citation: Phys. Chem. Chem. Phys., 2018,20, 2363-2372
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    A charge polarization model for the metal-specific activity of superoxide dismutases

    A. Barwinska-Sendra, A. Baslé, K. J. Waldron and S. Un, Phys. Chem. Chem. Phys., 2018, 20, 2363
    DOI: 10.1039/C7CP06829H

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