作为原子转移反应中的新活性氧化剂的一种单核非血 (III) -水化合物
Muniyandi Sankaralingam1, Yong-Min Lee1, Deepika G Karmalkar1
1Department of Chemistry and Nano Science , Ewha Womans University , Seoul 03760 , Korea.
Journal of the American Chemical Society
|October 2, 2018
概括
这项研究引入了一种新的 (III) -水复合物,可以有效地执行原子转移反应. 这种金属-水化合物与其氧对应物相比具有更高的反应性,为原子抽取提供了新的途径.
科学领域:
- 无机化学
- 催化剂
- 反应机制
背景情况:
- 金属-水化合物在原子转移 (HAT) 反应中通常不如金属-化合物.
- 在HAT中金属复合物的反应性受其氧化还原潜力的影响.
- 了解HAT的机械路径对于催化剂设计至关重要.
研究的目的:
- 合成和表征一个单核非血Mn (III) -水化合物.
- 研究原子转移 (HAT) 复合物的能力.
- 将Mn (III) - 水复合物的反应性和机制与其Mn (III) - 水氧类型进行比较.
主要方法:
- [dpaq) Mn (III) ]2+ (1) 和 [dpaq) Mn (III) ]2+ (2) 的合成和表征
- 电化学研究以确定一个电子的还原潜力 (Ered).
- 用各种基质探测HAT机制的动力学研究.
主要成果:
- (III) - 水复合物 (1) 的HAT反应性明显高于 (III) - 水氧复合物 (2).
- 与复合体 2 相比,复合体 1 的降解潜力更高 (1.03 V 与 SCE 相比),从而促进了 HAT.
- 复合体1的HAT机制在顺序电子-质子转移和协同质子-合电子转移之间有所变化,这取决于基质的氧化潜力.
结论:
- 金属-水复合物可以作为有效的H原子抽象试剂,挑战以前的假设.
- (III) - 水复合物的增强反应性归因于其有利的氧化还原潜力.
- 这项工作提供了第一个金属-水复合物的例子,作为一种强大的H原子抽象剂.
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