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Phys Chem Chem Phys. 2014 Jun 28;16(24):12067-72. doi: 10.1039/c3cp54946a.

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

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Institut de Chimie Moléculaire et des Matériaux d'Orsay, UMR 8182, Univ. Paris-Sud and CNRS, F-91405 Orsay, France.


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(II)-Ni(II) modular assembly with 450 nm visible light in the presence of a sacrificial electron donor accomplishes the reduction of CO2 into CO and H2 in a ratio of 2.7 to 1.

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