对于N组转移化学相关的铁-体物种的表征
Diana A Iovan1, Theodore A Betley1
1Department of Chemistry and Chemical Biology, Harvard University , 12 Oxford Street, Cambridge, Massachusetts 02138, United States.
Journal of the American Chemical Society
|January 21, 2016
概括
这项研究合成了一种新型的铁复合物,该复合物与酸反应,形成终端或桥梁的imido物种. 这些铁基复合物显示为N组转移反应和C-H氨化催化剂的潜力.
科学领域:
- 有机金属化学
- 协调化学
- 催化剂
背景情况:
- 铁复合物在各种催化转化中至关重要.
- 了解铁的反应性是开发新催化系统的关键.
- 硬质阻碍可以影响金属复合物的稳定性和反应性.
研究的目的:
- 合成和表征新型的三基替代二甲二铁复合物.
- 调查这些复合物的与酸的反应性,形成铁的imido物种.
- 在N组转移和C-H氨基化反应中探索由此产生的铁胺复合物的催化潜力.
主要方法:
- 一个三基替代的二氧化二铁 (II) 复合物的合成.
- 与各种酸发生反应,形成终端和桥梁铁模复合物.
- 用于结构和电子特征的Mössbauer光谱和X射线晶体学.
- 用SQUID磁力测量和固态磁力测量来确定磁性.
- 在现场监测以观察催化中间体.
主要成果:
- 成功合成了可以通过固体接入的三基替代的二氧化二铁 (II) 复合物.
- 形成两种不同的铁像素产物:一个终端铁像素和一个桥梁二铁像素,取决于酸结构.
- 铁模物种的电子结构和磁性特性,包括高旋转的Fe (III) 中心.
- 证明桥梁二铁像素作为一个有能力的N组转移试剂和C-H氨化中的催化活性物种.
结论:
- 合成的铁复合物提供了可调节反应的多种铁体物种.
- 在HAA和N组转移反应中,桥梁二铁模态复合体表现出催化活性.
- 这些发现凸显了铁胺复合物作为有机合成中的多功能催化剂的潜力.
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