mackinawit支持的C1底物还原成益生元相关前体

IF 3.1 Q2 CHEMISTRY, MULTIDISCIPLINARY
Dr. Mario Grosch, Dr. Martin T. Stiebritz, Dr. Robert Bolney, Mario Winkler, Eric Jückstock, Hannah Busch, Sophia Peters, Dr. Alexander F. Siegle, Prof. Joris van Slageren, Prof. Markus Ribbe, Prof. Yilin Hu, Prof. Oliver Trapp, Prof. Christian Robl, Prof. Wolfgang Weigand
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引用次数: 3

摘要

与其他硫化铁相比,Mackinawite具有独特的结构性质和反应活性。在这里,我们提供了在原始条件下mackinawite支持的KCN还原成各种还原性化合物的证据。我们提出了一种基于去质子化的mackinawite -SH表面基团对HCN碳原子亲核攻击的反应机理。底物的初始结合和随后的还原事件得到DFT计算和使用其他底物(如KSCN、KOCN和CS2)的进一步实验的支持。到目前为止,CN−转化为CH4和NH3仅限于氮酶辅助因子或分子Fe-CN配合物。我们的研究为在环境条件下麦金酸支持的C−N键的裂解提供了证据,这为研究麦金酸支持的反应的其他底物开辟了新的途径,同时揭示了这类反应与地球上生命起源的相关性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Mackinawite-Supported Reduction of C1 Substrates into Prebiotically Relevant Precursors

Mackinawite-Supported Reduction of C1 Substrates into Prebiotically Relevant Precursors

Mackinawite has unique structural properties and reactivities when compared to other iron sulfides. Herein we provide evidence for the mackinawite-supported reduction of KCN into various reduced compounds under primordial conditions. We proposed a reaction mechanism based on the nucleophilic attack by the deprotonated mackinawite -SH surface groups at the carbon atom of HCN. The initial binding of the substrate and the subsequent reduction events are supported by DFT calculations and further experiments using other substrates, such as KSCN, KOCN and CS2. Until now, conversion of CN into CH4 and NH3 has been limited to nitrogenase cofactors or molecular Fe-CN complexes. Our study provides evidence for mackinawite-supported cleavage of the C−N bond under ambient conditions, which opens new avenues for investigation of other substrates for mackinawite-supported reactions while shedding light on the relevance of this type of reaction to the origin of life on Earth.

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