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紫外光驱动的类生命合成铁硫簇。

UV-light-driven prebiotic synthesis of iron-sulfur clusters.

机构信息

CIBIO, University of Trento, via Sommarive 9, 38123 Povo, Italy.

Chemistry, School of Mathematics and Physical Sciences, University of Hull, Hull HU6 7RX, UK.

出版信息

Nat Chem. 2017 Dec;9(12):1229-1234. doi: 10.1038/nchem.2817. Epub 2017 Jul 10.

Abstract

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.

摘要

铁硫簇是古老的辅因子,在新陈代谢中起着至关重要的作用,可能对导致生命出现的前生物化学产生了影响。然而,在原始地球上是否可以合成铁硫簇还不清楚。早期地球上溶解的铁主要以还原态的亚铁形式存在,但亚铁离子本身无法形成多核铁硫簇。同样,游离的硫化物可能不易获得。在这里,我们证明了紫外光通过亚铁离子的光氧化和有机硫醇的光解,驱动[2Fe-2S]和[4Fe-4S]簇的合成。铁硫簇与广泛的含半胱氨酸肽配位,并被其稳定,铁硫簇-肽复合物的组装可以在模型原细胞内进行,这个过程与现存的途径相似。我们的实验表明,铁硫簇可能很容易在早期地球上形成,从而促进了依赖铁硫簇的新陈代谢的出现。

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UV-light-driven prebiotic synthesis of iron-sulfur clusters.紫外光驱动的类生命合成铁硫簇。
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A [3Fe-4S] cluster is required for tRNA thiolation in archaea and eukaryotes.古菌和真核生物中tRNA硫醇化需要一个[3铁-4硫]簇。
Proc Natl Acad Sci U S A. 2016 Nov 8;113(45):12703-12708. doi: 10.1073/pnas.1615732113. Epub 2016 Oct 24.
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Mössbauer spectroscopy of Fe/S proteins.铁硫蛋白的穆斯堡尔光谱学
Biochim Biophys Acta. 2015 Jun;1853(6):1395-405. doi: 10.1016/j.bbamcr.2014.12.005. Epub 2014 Dec 10.

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