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通过改变催化中心生成稳定的超分子析氢光催化剂。

Generation of a stable supramolecular hydrogen evolving photocatalyst by alteration of the catalytic center.

作者信息

Mengele Alexander K, Kaufhold Simon, Streb Carsten, Rau Sven

机构信息

University of Ulm, Institute of Inorganic Chemistry Materials and Catalysis, Albert-Einstein-Allee 11, 89081 Ulm, Germany.

出版信息

Dalton Trans. 2016 Apr 21;45(15):6612-8. doi: 10.1039/c6dt00130k.

DOI:10.1039/c6dt00130k
PMID:26965197
Abstract

A new dyad consisting of a Ru(II) chromophore, a tetrapyridophenazine bridging ligand and a Rh(Cp*)Cl catalytic center, [Ru(tbbpy)2(tpphz)Rh(Cp*)Cl]Cl(PF6)2, acts as durable photocatalyst for hydrogen production from water. Catalytic activity is observed for more than 650 hours. Electrochemical investigations reveal that up to two electrons can be transferred to the catalytic center by a thermodynamically favorable intramolecular process, which has so far not been reported for similar tpphz based supramolecular photocatalysts. Additionally, mercury poisoning tests indicate that the new dyad works as a homogeneous photocatalyst.

摘要

一种由钌(II)发色团、四吡啶并菲桥连配体和铑(Cp*)Cl催化中心组成的新型二元体系[Ru(tbbpy)2(tpphz)Rh(Cp*)Cl]Cl(PF6)2,可作为从水中制氢的持久光催化剂。观察到催化活性持续超过650小时。电化学研究表明,通过热力学有利的分子内过程,最多可将两个电子转移到催化中心,这在基于tpphz的类似超分子光催化剂中尚未见报道。此外,汞中毒测试表明该新型二元体系作为均相光催化剂起作用。

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