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通过Pd(0)-氨酸二氨酸复合物减少氧气
Kyle T Horak1, Theodor Agapie1
1Division of Chemistry and Chemical Engineering, California Institute of Technology , 1200 East California Boulevard MC 127-72, Pasadena, California 91125, United States.
Journal of the American Chemical Society
|March 8, 2016
概括
一个新的复合物与基连接物有效地减少各种小分子,包括氧气. 这种金属合反应突出了连接物
科学领域:
- 有机金属化学
- 协调化学
背景情况:
- 新型配体的开发对于促进催化是至关重要的.
- 在金属复合体中提供独特的反应途径.
研究的目的:
- 合成和描述一种具有基部分的新型p-terphenyl diphosphine连接物.
- 研究由此产生的金属复合物的反应性,特别是小分子.
- 通过二坐标-化复合物来阐明二氧化降解的机制.
主要方法:
- 一种含有基核的p-二联体的合成.
- 与Ni(0) 和Pd(0) 前体发生金属化反应,形成金属复合物.
- 通过单金属化和减少制备2坐标Pd(0)-化合物.
- 用各种小分子进行反应性研究,包括O2,NO,N2O和有机氧化物.
- 使用对照化合物和低温研究的机制研究.
主要成果:
- 合成了一种含有基的新型二素配体.
- 形成了伪四面体的Ni{0}和Pd{0}-子复合体.
- 一个2坐标的Pd(0)-基复合体表现出对小分子的金属合反应性.
- 这种复合物量减少了O2,NO,N2O和有机氧化物,产生了Pd(0) - 子产物.
- 二氧化物还原过程通过一个eta(2) - peroxo中间体,然后是连接物氧化.
结论:
- 复合体中的基部分在小分子激活和减少中起着关键作用.
- 双坐标Pd(0) - 胺复合物是各种基质的强有力的减少剂.
- 二氧化激活是一种基于Pd的内部球体过程,基配体参与后续的还原步骤.
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