A radical pathway for organic phosphorylation during schreibersite corrosion with implications for the origin of life

A radical pathway for organic phosphorylation during schreibersite corrosion with implications for the origin of life
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DOI:
10.1016/j.gca.2006.12.018
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发表时间:
2007-04-01
影响因子:
5
通讯作者:
Lauretta, Dante S.
Lauretta, Dante S.
中科院分区:
地球科学1区
文献类型:
--
作者:
Pasek, Matthew A.;Dworkin, Jason P.;Lauretta, Dante S.

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磷酸化化合物(例如,DNA,RNA,磷脂和许多辅酶)对生物化学至关重要。因此,它们的起源是生命起源研究的首要兴趣。陨石矿物石((Fe,Ni)(3)P)的腐蚀可能对磷酸化生物分子的起源有重要贡献。采用核磁共振谱、质谱和电子顺磁共振谱分析了人工合成钙铝尖晶石在不同溶液中的腐蚀行为。这些方法表明钙钛矿的腐蚀是通过自由基反应生成亚磷酸根((PO 32-)-P-.)在水溶液中这些自由基可以形成活化的多磷酸盐,并且可以磷酸化有机化合物如乙酸盐以形成膦酸盐和有机磷酸酯(3%总产率)。磷酸盐(O3 P-C)在碳质陨石Murchison的有机磷库存中发现。虽然膦酸盐在生物化学中很少见,但早期地球上普遍存在的腐蚀性铁陨石可能为生命的起源提供了有机磷化合物的来源,并可能导致有机磷酸盐作为早期进化的产物。(c)2007爱思唯尔有限公司保留所有权利。
Phosphorylated compounds (e.g., DNA, RNA, phospholipids, and many coenzymes) are critical to biochemistry. Thus, their origin is of prime interest to origin of life studies. The corrosion of the meteoritic mineral schreibersite ((Fe,Ni)(3)P) may have significantly contributed to the origin of phosphorylated biomolecules. Corrosion of synthetic schreibersite in a variety of solutions was analyzed by nuclear magnetic resonance spectroscopy, mass spectrometry, and electron paramagnetic resonance spectroscopy. These methods suggest a free-radical reaction pathway for the corrosion of schreibersite to form phosphite radicals ((PO32-)-P-.) in aqueous solution. These radicals can form activated polyphosphates and can phosphorylate organic compounds such as acetate to form phosphonates and organophosphates (3% total yield). Phosphonates (O3P-C) are found in the organic P inventory of the carbonaceous meteorite Murchison. While phosphonates are rare in biochemistry, the ubiquity of corroding iron meteorites on the early Earth could have provided a source of organic phosphorous compounds for the origin of life, and may have led to the role of organophosphates as a product of early evolution. (c) 2007 Elsevier Ltd. All rights reserved.