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一个双核铁 (II) 硫化物复合体与O2反应,产生硫酸盐:与硫化物二氧化基酶的相关性

Jasper G Ballot¹, Maxime A Siegler¹, Yisong Guo²

¹Department of Chemistry, The Johns Hopkins University, Baltimore, Maryland 21218, United States.

Journal of the American Chemical Society

|March 12, 2026

概括

这项研究报告了第一个合成铁 (II) - 硫化物复合物,模仿生物硫化物氧化. 该复合物与氧气发生反应,形成二铁 (III) 氧桥性物种,揭示了铁硫集群生物化学的洞察力.

科学领域:

生物有机化学生物有机化学
协调化学协调化学
生物化学生物化学

背景情况:

硫化物 (RSSH) 在涉及铁的生物过程中至关重要,例如铁硫集群组装和硫氧化.
通过ETHE1等非血铁酶氧化的机制尚不清楚.
缺乏合成类似物来研究铁介导的硫化物转化.

研究的目的:

为了合成和表征一种新的铁(II) - 硫化物复合物.
为了研究这个复合体与分子氧的反应性.
阐明与生物系统相关的铁介导硫酸氧化机制.

主要方法:

使用X射线衍射,UV视,NMR和Mössbauer光谱学合成和表征一个阿达曼硫酸盐和一个双核铁 (II) 复合物.
研究铁 (II) 复合物与O2的反应.
用18O2和H218O进行同位素标记研究,并进行ESI-MS分析.

主要成果:

一种稳定的铁(II) - 亚达曼甲硫化物复合物,[(FeII(Me3TACN)) 2(μ2-SSAd) 3[OTf],被合成并得到了充分的特征.
与O2的反应产生了二铁(III) 氧桥复合体,[(FeIII(Me3TACN)) 2(μ-O) (((μ2-SO4) (((μ2-SO3Ad) ][OTf],以及硫酸盐.
同位素标记证实了硫酸盐生产的以铁为中心的S-氧化机制.

结论:

合成的铁(II) - 基硫化物复合物作为一种有价值的合成模拟物用于研究硫化物生物化学.
这项研究提供了对铁介导的硫化物氧化机制的洞察,反映了酶途径.
这项工作促进了对硫代谢和铁硫集团化学的理解.

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