Photoproduction of Hydrogen by Decamethylruthenocene Combined with Electrochemical Recycling

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• 作者：Lucie Rivier ; Dr. Pekka Peljo ; Laurent A. C. Vannay ; Gré ; goire C. Gschwend ; Dr. Manuel A. Mé ; ndez ; Prof. Clé ; mence Corminboeuf ; Dr. Micheá ; l D. Scanlon and Prof. Hubert H. Girault
• 刊名：Angewandte Chemie
• 出版年：2017
• 出版时间：February 20, 2017
• 年：2017
• 卷：129
• 期：9
• 页码：2364-2367
• 全文大小：1209K
• ISSN：1521-3757

文摘

The photoinduced hydrogen evolution reaction (HER) by decamethylruthenocene, Cp₂*Ru^II (Cp*=C₅Me₅), is reported. The use of a metallocene to photoproduce hydrogen is presented as an alternative strategy to reduce protons without involving an additional photosensitizer. The mechanism was investigated by (spectro)electrochemical and spectroscopic (UV/Vis and ¹H NMR) measurements. The photoactivated hydride involved was characterized spectroscopically and the resulting [Cp₂*Ru^III]⁺ species was electrochemically regenerated in situ on a fluorinated tin oxide electrode surface. A promising internal quantum yield of 25 % was obtained. Optimal experimental conditions— especially the use of weakly coordinating solvent and counterions—are discussed.