Journal
NATURE CHEMISTRY
Volume 9, Issue 12, Pages 1229-1234Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2817
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Funding
- Simons Foundation [290360, 290363, 290362, 290358]
- Armenise-Harvard Foundation
- COST action [CM1304]
- University of Hull
- Medical Research Council [MC_UP_A024_1009] Funding Source: researchfish
- MRC [MC_UP_A024_1009] Funding Source: UKRI
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Iron-sulfur clusters are ancient cofactors that play a fundamental role in metabolism and may have impacted the prebiotic chemistry that led to life. However, it is unclear whether iron-sulfur clusters could have been synthesized on prebiotic Earth. Dissolved iron on early Earth was predominantly in the reduced ferrous state, but ferrous ions alone cannot form polynuclear iron-sulfur clusters. Similarly, free sulfide may not have been readily available. Here we show that UV light drives the synthesis of [2Fe-2S] and [4Fe-4S] clusters through the photooxidation of ferrous ions and the photolysis of organic thiols. Iron-sulfur clusters coordinate to and are stabilized by a wide range of cysteine-containing peptides and the assembly of iron-sulfur cluster-peptide complexes can take place within model protocells in a process that parallels extant pathways. Our experiments suggest that iron-sulfur clusters may have formed easily on early Earth, facilitating the emergence of an iron-sulfur-cluster-dependent metabolism.
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