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Photoreduction of inorganic carbon(+IV) by elemental sulfur: Implications for prebiotic synthesis in terrestrial hot springs
Science Advances ( IF 11.7 ) Pub Date : 2020-11-18 , DOI: 10.1126/sciadv.abc3687
Yanzhang Li 1, 2 , Yan Li 1, 2 , Yi Liu 1, 2 , Yifu Wu 1, 2 , Junqi Wu 1, 2 , Bin Wang 3 , Huan Ye 1, 2 , Haoning Jia 1, 2 , Xiao Wang 1, 2 , Linghui Li 1, 2 , Meixiang Zhu 1, 2 , Hongrui Ding 1, 2 , Yong Lai 1, 2 , Changqiu Wang 1, 2 , Jeffrey Dick 4 , Anhuai Lu 1, 2, 4
Affiliation  

Terrestrial hydrothermal systems have been proposed as alternative birthplaces for early life but lacked reasonable scenarios for the supply of biomolecules. Here, we show that elemental sulfur (S0), as the dominant mineral in terrestrial hot springs, can reduce carbon dioxide (CO2) into formic acid (HCOOH) under ultraviolet (UV) light below 280 nm. The semiconducting S0 is indicated to have a direct bandgap of 4.4 eV. The UV-excited S0 produces photoelectrons with a highly negative potential of −2.34 V (versus NHE, pH 7), which could reduce CO2 after accepting electrons from electron donors such as reducing sulfur species. Simultaneously, UV light breaks sulfur bonds, benefiting the adsorption of charged carbonates onto S0 and assisting their photoreduction. Assuming that terrestrial hot springs covered 1% of primitive Earth’s surface, S0 at 10 μM could have produced maximal 109 kg/year HCOOH within 10-cm-thick photic zones, underlying its remarkable contributions to the accumulation of prebiotic biomolecules.



中文翻译:

元素硫对无机碳(+ IV)的光还原作用:对陆地温泉中益生元合成的影响

有人提出将陆地热液系统作为早期生活的替代发源地,但缺乏提供生物分子的合理方案。在这里,我们表明元素硫(S 0)作为陆地温泉中的主要矿物,可以在280 nm以下的紫外线(UV)下将二氧化碳(CO 2)还原为甲酸(HCOOH)。半导体S 0被示为具有4.4eV的直接带隙。紫外线激发的S 0产生具有-2.34 V的高负电势(相对于NHE,pH 7)的光电子,这可以减少CO 2接受来自电子供体的电子,例如还原硫物种。同时,紫外线会破坏硫键,有利于带电荷的碳酸盐在S 0上的吸附并有助于其光还原。假设地面温泉覆盖了原始地球表面的1%,则10μM的S 0可能在10厘米厚的光生带内产生最大10 9 kg /年的HCOOH,这是其对益生元生物分子积累的显着贡献。

更新日期:2020-11-19
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