A Supramolecularly Activated Radical Cation for Accelerated Catalytic Oxidation

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• 作者：Yang Jiao ; Wan-Lu Li ; Dr. Jiang-Fei Xu ; Dr. Guangtong Wang ; Prof. Jun Li ; Prof. Zhiqiang Wang and Prof. Xi Zhang
• 刊名：Angewandte Chemie International Edition
• 出版年：2016
• 出版时间：July 25, 2016
• 年：2016
• 卷：55
• 期：31
• 页码：8933-8937
• 全文大小：2840K
• ISSN：1521-3773

文摘

Tuning the activity of radicals is crucial for radical reactions and radical-based materials. Herein, we report a supramolecular strategy to accelerate the Fenton reaction through the construction of supramolecularly activated radical cations. As a proof of the concept, cucurbit[7]uril (CB[7]) was introduced, through host–guest interactions, onto each side of a derivative of 1,4-diketopyrrolo[3,4-c]pyrrole (DPP), a model dye for Fenton oxidation. The DPP radical cation, the key intermediate in the oxidation process, was activated by the electrostatically negative carbonyl groups of CB[7]. The activation induced a drastic decrease in the apparent activation energy and greatly increased the reaction rate. This facile supramolecular strategy is a promising method for promoting radical reactions. It may also open up a new route for the catalytic oxidation of organic pollutants for water purification and widen the realm of supramolecular catalysis.