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使用具有钌(II)-铼(I)配合物光催化剂的光阴极和氧化钴/钽酸氮光阳极将二氧化碳光电化学还原与水氧化耦合。

Photoelectrochemical Reduction of CO Coupled to Water Oxidation Using a Photocathode with a Ru(II)-Re(I) Complex Photocatalyst and a CoO/TaON Photoanode.

作者信息

Sahara Go, Kumagai Hiromu, Maeda Kazuhiko, Kaeffer Nicolas, Artero Vincent, Higashi Masanobu, Abe Ryu, Ishitani Osamu

机构信息

Department of Chemistry, School of Science, Tokyo Institute of Technology , O-okayama 2-12-1-NE-1, Meguro-ku, Tokyo 152-8550, Japan.

Laboratoire de Chimie et Biologie des Métaux, Université Grenoble Alpes , CNRS UMR 5249, CEA, F-38000 Grenoble, France.

出版信息

J Am Chem Soc. 2016 Oct 26;138(42):14152-14158. doi: 10.1021/jacs.6b09212. Epub 2016 Oct 14.

Abstract

Photoelectrochemical CO reduction activity of a hybrid photocathode, based on a Ru(II)-Re(I) supramolecular metal complex photocatalyst immobilized on a NiO electrode (NiO-RuRe), was confirmed in an aqueous electrolyte solution. Under half-reaction conditions, the NiO-RuRe photocathode generated CO with high selectivity, and its turnover number for CO formation reached 32 based on the amount of immobilized RuRe. A photoelectrochemical cell comprising a NiO-RuRe photocathode and a CoO/TaON photoanode showed activity for visible-light-driven CO reduction using water as a reductant to generate CO and O, with the assistance of an external electrical (0.3 V) and chemical (0.10 V) bias produced by a pH difference. This is the first example of a molecular and semiconductor photocatalyst hybrid-constructed photoelectrochemical cell for visible-light-driven CO reduction using water as a reductant.

摘要

基于固定在NiO电极(NiO-RuRe)上的Ru(II)-Re(I)超分子金属配合物光催化剂的混合光阴极在水性电解质溶液中的光电化学CO还原活性得到了证实。在半反应条件下,NiO-RuRe光阴极以高选择性生成CO,基于固定的RuRe的量,其CO形成的周转数达到32。由NiO-RuRe光阴极和CoO/TaON光阳极组成的光电化学电池在pH差产生的外部电(0.3 V)和化学(0.10 V)偏压的辅助下,表现出使用水作为还原剂进行可见光驱动的CO还原以生成CO和O的活性。这是第一个使用水作为还原剂的分子和半导体光催化剂混合构建的用于可见光驱动的CO还原的光电化学电池的例子。

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