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Desulfovibrio gigas ferredoxin II: redox structural modulation of the [3Fe–4S] cluster

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Abstract

Desulfovibrio gigas ferredoxin II (DgFdII) is a small protein with a polypeptide chain composed of 58 amino acids, containing one Fe3S4 cluster per monomer. Upon studying the redox cycle of this protein, we detected a stable intermediate (FdIIint) with four 1H resonances at 24.1, 20.5, 20.8 and 13.7 ppm. The differences between FdIIox and FdIIint were attributed to conformational changes resulting from the breaking/formation of an internal disulfide bridge. The same 1H NMR methodology used to fully assign the three cysteinyl ligands of the [3Fe–4S] core in the oxidized state (DgFdIIox) was used here for the assignment of the same three ligands in the intermediate state (DgFdIIint). The spin-coupling model used for the oxidized form of DgFdII where magnetic exchange coupling constants of around 300 cm−1 and hyperfine coupling constants equal to 1 MHz for all the three iron centres were found, does not explain the isotropic shift temperature dependence for the three cysteinyl cluster ligands in DgFdIIint. This study, together with the spin delocalization mechanism proposed here for DgFdIIint, allows the detection of structural modifications at the [3Fe-4S] cluster in DgFdIIox and DgFdIIint.

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Abbreviations

Dg :

Desulfovibrio gigas

Fd:

Ferredoxin

NOE:

Nuclear Overhauser effect

NOESY:

Nuclear Overhauser enhancement spectroscopy

SRB:

Sulfate-reducing bacteria

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Acknowledgements

We would like to thank Ludwig Krippahl for his help with the computer software provided by him and used in this work. This work was supported by Fundação para a Ciência e Tecnologia and COST D2 1.

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Authors and Affiliations

  1. FCMA, CCMAR, Universidade do Algarve, Campus de Gambelas, 8005-139, Faro, Portugal

    Pedro M. Rodrigues

  2. REQUIMTE, Departamento de Química, Centro de Química Fina e Biotecnologia, Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa, 2829-516, Caparica, Portugal

    Anjos L. Macedo, Isabel Moura & José J. G. Moura

  3. Departamento de Química, Universidade de Aveiro, 3810, Aveiro, Portugal

    Brian J. Goodfellow

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  1. Pedro M. Rodrigues
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  2. Anjos L. Macedo
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  4. Isabel Moura
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  5. José J. G. Moura
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Correspondence to José J. G. Moura.

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Rodrigues, P.M., Macedo, A.L., Goodfellow, B.J. et al. Desulfovibrio gigas ferredoxin II: redox structural modulation of the [3Fe–4S] cluster. J Biol Inorg Chem 11, 307–315 (2006). https://doi.org/10.1007/s00775-005-0077-2

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