Carbon dioxide reduction via light activation of a ruthenium-Ni(cyclam) complex

被引：47
作者：
Herrero, Christian [1 ,2 ]
Quaranta, Annamaria [3 ]
El Ghachtouli, Sanae [3 ]
Vauzeilles, Boris [4 ,5 ]
Leibl, Winfried [3 ]
Aukauloo, Ally [1 ,2 ,3 ]
机构：
[1] Univ Paris 11, Inst Chim Mol & Mat Orsay, UMR 8182, F-91405 Orsay, France
[2] CNRS, F-91405 Orsay, France
[3] CEA, IBiTecS, Serv Bioenerget Biol Struct & Mecanismes, UMR 8221, F-91191 Gif Sur Yvette, France
[4] Ctr Rech Gif, ICSN, F-91198 Gif Sur Yvette, France
[5] Univ Paris 11, ICMMO, LG2M, F-91405 Orsay, France
来源：
PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2014年 / 16卷 / 24期
关键词：
CO2; REDUCTION; PHOTOCHEMICAL REDUCTION; ENERGY-CONVERSION; AQUEOUS-SOLUTION; H+ BINDING; NICKEL(II); CHEMISTRY; CATALYST; WATER; THERMODYNAMICS;
D O I：
10.1039/c3cp54946a
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
In this paper we report the synthesis of a chromophore-catalyst assembly designed for the photoreduction of carbon dioxide. The chromophore unit is made up of a ruthenium trisbipyridyl-like unit covalently attached to a nickel cyclam (cyclam = 1,4,8,11-tetraazacyclotetradecane) via a triazole ring. The intramolecular electron transfer activation of the catalyst unit by visible light was studied by nanosecond flash photolysis and EPR spectroscopy. In aqueous solutions (pH = 6.5), activation of the Ru-broken vertical bar broken vertical bar-Ni-broken vertical bar broken vertical bar modular assembly with 450 nm visible light in the presence of a sacrificial electron donor accomplishes the reduction of CO2 into CO and H-2 in a ratio of 2.7 to 1.
引用
收藏
页码：12067 / 12072
页数：6
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