持続可能な触媒の設計(Designing sustainable catalysts)

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2024-02-23 インペリアル・カレッジ・ロンドン(ICL)

触媒は社会に不可欠な化学反応を支えるが、持続可能性を高めるための研究が進む。特に電子移動に依存する分子触媒に対し、表面への固定化が有望であり、これにより廃棄物が減り、穏やかな条件での産業的なプロセスが可能となる。インペリアル大学のチームは、フィルム電気化学と電子スピン共鳴を組み合わせて、反応中のラジカルをリアルタイムで追跡し、触媒の効率的な電子移動に焦点を当てた。

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表面固定化触媒のラジカル中間体を追跡するオペランドフィルム電気化学EPR分光法 Operando film-electrochemical EPR spectroscopy tracks radical intermediates in surface-immobilized catalysts

Maryam Seif-Eddine,Samuel J. Cobb,Yunfei Dang,Kaltum Abdiaziz,Mark A. Bajada,Erwin Reisner & Maxie M. Roessler
Nature Chemistry  Published:14 February 2024
DOI:https://doi.org/10.1038/s41557-024-01450-y

Abstract

The development of surface-immobilized molecular redox catalysts is an emerging research field with promising applications in sustainable chemistry. In electrocatalysis, paramagnetic species are often key intermediates in the mechanistic cycle but are inherently difficult to detect and follow by conventional in situ techniques. We report a new method, operando film-electrochemical electron paramagnetic resonance spectroscopy (FE-EPR), which enables mechanistic studies of surface-immobilized electrocatalysts. This technique enables radicals formed during redox reactions to be followed in real time under flow conditions, at room temperature and in aqueous solution. Detailed insight into surface-immobilized catalysts, as exemplified here through alcohol oxidation catalysis by a surface-immobilized nitroxide, is possible by detecting active-site paramagnetic species sensitively and quantitatively operando, thereby enabling resolution of the reaction kinetics. Our finding that the surface electron-transfer rate, which is of the same order of magnitude as the rate of catalysis (accessible from operando FE-EPR), limits catalytic efficiency has implications for the future design of better surface-immobilized catalysts.

持続可能な触媒の設計(Designing sustainable catalysts)

0500化学一般
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