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模拟早期地球上闪电引发的电化学过程。

Mimicking lightning-induced electrochemistry on the early Earth.

作者信息

Jiang Haihui Joy, Underwood Thomas C, Bell Jeffrey G, Lei Jonathan, Gonzales Joe C, Emge Lukas, Tadese Leah G, Abd El-Rahman Mohamed K, Wilmouth David M, Brazaca Lais C, Ni Gigi, Belding Lee, Dey Supriya, Ashkarran Ali Akbar, Nagarkar Amit, Nemitz Markus P, Cafferty Brian J, Sayres David S, Ranjan Sukrit, Crocker Daniel R, Anderson James G, Sasselov Dimitar D, Whitesides George M

机构信息

Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138.

Department of Astronomy, Harvard University, Cambridge, MA 02138.

出版信息

Proc Natl Acad Sci U S A. 2024 Aug 6;121(32):e2400819121. doi: 10.1073/pnas.2400819121. Epub 2024 Jul 29.

Abstract

To test the hypothesis that an abiotic Earth and its inert atmosphere could form chemically reactive carbon- and nitrogen-containing compounds, we designed a plasma electrochemical setup to mimic lightning-induced electrochemistry under steady-state conditions of the early Earth. Air-gap electrochemical reactions at air-water-ground interfaces lead to remarkable yields, with up to 40 moles of carbon dioxide being reduced into carbon monoxide and formic acid, and 3 moles of gaseous nitrogen being fixed into nitrate, nitrite, and ammonium ions, per mole of transmitted electrons. Interfaces enable reactants (e.g., minerals) that may have been on land, in lakes, and in oceans to participate in radical and redox reactions, leading to higher yields compared to gas-phase-only reactions. Cloud-to-ground lightning strikes could have generated high concentrations of reactive molecules locally, establishing diverse feedstocks for early life to emerge and survive globally.

摘要

为了验证非生物地球及其惰性大气能够形成具有化学反应性的含碳和含氮化合物这一假设,我们设计了一种等离子体电化学装置,以模拟早期地球稳态条件下由闪电引发的电化学过程。气-水-地界面处的气隙电化学反应产生了可观的产量,每摩尔传输电子可使多达40摩尔的二氧化碳被还原为一氧化碳和甲酸,3摩尔气态氮被固定为硝酸盐、亚硝酸盐和铵离子。界面使得可能存在于陆地、湖泊和海洋中的反应物(如矿物质)能够参与自由基和氧化还原反应,与仅气相反应相比,产量更高。云对地的雷击可能在局部产生高浓度的活性分子,为早期生命在全球范围内的出现和生存建立了多样的原料。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8d73/11317556/40e76858cd82/pnas.2400819121fig01.jpg

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