将单氧原子桥梁双金属系统推向右边:一个加密封装的Co-O-Co单元
Julia M Stauber1, Eric D Bloch1,2, Konstantinos D Vogiatzis3
1Department of Chemistry, Massachusetts Institute of Technology , Cambridge, Massachusetts 02139, United States.
Journal of the American Chemical Society
|November 13, 2015
概括
这项研究引入了形成独特Co-O-Co核心的双复合物. 这种复合物作为氧化剂和催化剂,表现出高效的氧原子转移反应.
科学领域:
- 无机化学
- 协调化学
- 催化剂
背景情况:
- 迪科巴尔特复合物因其催化性质而有意义.
- 了解金属与金属的相互作用和氧化状态对于设计新的催化剂至关重要.
研究的目的:
- 合成和表征一种具有Co (II) 离子共面排列的新型二复合物.
- 研究Co-O-Co核的形成及其反应性.
- 探索二系统作为氧化剂和催化剂的催化应用.
主要方法:
- 双复合物的合成和表征.
- 用于氧化状态的X射线吸收光谱 (XAS).
- 通过二次扰动理论 (CASPT2) 进行多参照完整活跃空间计算 (CASSCF).
- 包括氧化反应和催化试验的反应性研究.
主要成果:
- 合成了一种二二复合物,Co2{mBDCA-5t) }{2-) (1),具有Co2{II}离子的对面排列.
- 与超氧化物反应产生了一种新的复合物,[Co2O(mBDCA-5t) ](2-) (2),具有线性Co-O-Co核心.
- 在两种复合物中,光谱和计算数据证实了的+2氧化状态.
- 复合体2向CO和H2表现出2电子的氧化行为,再生复合体1.
- 迪科巴尔特系统表现出与H2O2的催化酶活性.
结论:
- 该研究成功合成并描述了一种能够形成Co-O-Co核心的新型二复合物.
- 该复合物作为有效的2电子氧化剂和催化剂,表现出氧原子转移能力.
- 在催化和氧化反应中,这种二系统具有前景.
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