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

页码：12067 / 12072

页数：6

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