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通过单核非血铁复合物激活二氧化物:序列,和中间体

Jesse B Gordon¹, Avery C Vilbert², Ida M DiMucci²

¹Department of Chemistry , The Johns Hopkins University , 3400 North Charles Street , Baltimore , Maryland 21218 , United States.

Journal of the American Chemical Society

|October 25, 2019

概括

这项研究报告了由单核非血铁 (II) 复合物激活氧气,形成Fe^III-O-O-Fe^III和Fe^IV(O) 中介物. 这项工作证明了在铁氧化学中使用硫联体的可行性.

科学领域:

生物有机化学
有机金属化学
协调化学

背景情况:

非血铁复合物的二氧化激活对于生物过程和催化是至关重要的.
了解铁氧中间体的机制是设计高效催化剂的关键.
单核非铁系统为研究复杂反应性提供了简化模型.

研究的目的:

为了研究由单核非血铁 (II) 复合物与硫捐赠配体激活氧气.
描述产生的铁氧中间体,包括过氧和高价值铁氧物种.
探索这些中间体的反应性及其对催化物的影响.

主要方法:

使用UV-vis,Mössbauer,共振拉曼 (RR) 和X射线吸收 (XAS) 光谱的铁复合物的合成和表征.
与二氧化物低温反应以产生和分离反应性中间体.
频谱和反应性研究以阐明铁氧物种的结构和转变.

主要成果:

在与O_{2反应时形成酸结合 (氧) 铁复合物 (Fe^III₂(O₂).}
通过氧中间体的O-O键裂变生成一个Fe^IV(O) 种.
从Fe^IV(O) 种与H原子捐赠者的Fe^III(OH) 形成的观察.
在没有直接氧化硫的情况下证明稳定的Fe/O₂中间体.

结论:

这项研究提供了一个由单核非血铁 (II) 复合体激活氧气的罕见例子.
该研究成功地生成和表征了Fe^III-O-O-Fe^III和Fe^IV(O) 在同一反应中的物种.
这些发现突显了强度捐赠的硫联体在稳定反应性铁氧中间体中的作用.

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