Merging Two Functions in a Single Rh Catalyst System: Bimodular Conjugate for Light-Induced Oxidative Coupling,Journal of the American Chemical Society

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Merging Two Functions in a Single Rh Catalyst System: Bimodular Conjugate for Light-Induced Oxidative Coupling
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-10-30 , DOI: 10.1021/jacs.0c09982
Jinwoo Kim _{1,

2} , Dongwook Kim ₂ , Sukbok Chang _{1,

2}

Affiliation

A single molecular rhodium catalyst system (PC2-Cp#RhIII) bearing two functional domains for both photosensitization and C-H carbometalation was designed to enable an intramolecular redox process. The hypothesized charge-transfer species (PC2•--Cp#RhIV) was characterized by spectroscopic and electrochemical analyses. This photoinduced internal oxidation allows a facile access to the triplet state of the key post-transmetalation intermediate that readily undergoes C-C bond-forming reductive elimination with a lower activation barrier than in its singlet state, thus enabling catalytic C-H arylation and methylation processes.

中文翻译：

在单个 Rh 催化剂系统中合并两个功能：用于光诱导氧化偶联的双模共轭物

设计了一种单分子铑催化剂体系 (PC2-Cp#RhIII)，其具有用于光敏化和 CH 碳金属化的两个功能域，旨在实现分子内氧化还原过程。假设的电荷转移物质 (PC2•--Cp#RhIV) 通过光谱和电化学分析进行表征。这种光诱导的内部氧化可以很容易地进入关键的金属转移后中间体的三线态，该中间体很容易进行 CC 键形成还原消除，其活化势垒低于单线态，从而实现催化 CH 芳基化和甲基化过程。

更新日期：2020-10-30

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