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Spontaneous assembly of redox-active iron-sulfur clusters at low concentrations of cysteine

Author

Listed:
  • Sean F. Jordan

    (University College London)

  • Ioannis Ioannou

    (University College London)

  • Hanadi Rammu

    (University College London)

  • Aaron Halpern

    (University College London)

  • Lara K. Bogart

    (University College London)

  • Minkoo Ahn

    (University College London)

  • Rafaela Vasiliadou

    (University College London)

  • John Christodoulou

    (University College London)

  • Amandine Maréchal

    (University College London
    Institute of Structural and Molecular Biology, Birkbeck College)

  • Nick Lane

    (University College London)

Abstract

Iron-sulfur (FeS) proteins are ancient and fundamental to life, being involved in electron transfer and CO2 fixation. FeS clusters have structures similar to the unit-cell of FeS minerals such as greigite, found in hydrothermal systems linked with the origin of life. However, the prebiotic pathway from mineral surfaces to biological clusters is unknown. Here we show that FeS clusters form spontaneously through interactions of inorganic Fe2+/Fe3+ and S2− with micromolar concentrations of the amino acid cysteine in water at alkaline pH. Bicarbonate ions stabilize the clusters and even promote cluster formation alone at concentrations >10 mM, probably through salting-out effects. We demonstrate robust, concentration-dependent formation of [4Fe4S], [2Fe2S] and mononuclear iron clusters using UV-Vis spectroscopy, 57Fe-Mössbauer spectroscopy and 1H-NMR. Cyclic voltammetry shows that the clusters are redox-active. Our findings reveal that the structures responsible for biological electron transfer and CO2 reduction could have formed spontaneously from monomers at the origin of life.

Suggested Citation

  • Sean F. Jordan & Ioannis Ioannou & Hanadi Rammu & Aaron Halpern & Lara K. Bogart & Minkoo Ahn & Rafaela Vasiliadou & John Christodoulou & Amandine Maréchal & Nick Lane, 2021. "Spontaneous assembly of redox-active iron-sulfur clusters at low concentrations of cysteine," Nature Communications, Nature, vol. 12(1), pages 1-14, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26158-2
    DOI: 10.1038/s41467-021-26158-2
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    References listed on IDEAS

    as
    1. George W. Luther & Tim F. Rozan & Martial Taillefert & Donald B. Nuzzio & Carol Di Meo & Timothy M. Shank & Richard A. Lutz & S. Craig Cary, 2001. "Chemical speciation drives hydrothermal vent ecology," Nature, Nature, vol. 410(6830), pages 813-816, April.
    2. Kamila B. Muchowska & Sreejith J. Varma & Joseph Moran, 2019. "Synthesis and breakdown of universal metabolic precursors promoted by iron," Nature, Nature, vol. 569(7754), pages 104-107, May.
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