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Photo-generated dinuclear {Eu(II)}2 active sites for selective CO2 reduction in a photosensitizing metal-organic framework
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Photo-generated dinuclear {Eu(II)}2 active sites for selective CO2 reduction in a photosensitizing metal-organic framework
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Journal Article
Photo-generated dinuclear {Eu(II)}2 active sites for selective CO2 reduction in a photosensitizing metal-organic framework
2018
Overview
Photocatalytic reduction of CO
2
is a promising approach to achieve solar-to-chemical energy conversion. However, traditional catalysts usually suffer from low efficiency, poor stability, and selectivity. Here we demonstrate that a large porous and stable metal-organic framework featuring dinuclear Eu(III)
2
clusters as connecting nodes and Ru(phen)
3
-derived ligands as linkers is constructed to catalyze visible-light-driven CO
2
reduction. Photo-excitation of the metalloligands initiates electron injection into the nodes to generate dinuclear {Eu(II)}
2
active sites, which can selectively reduce CO
2
to formate in a two-electron process with a remarkable rate of 321.9 μmol h
−1
mmol
MOF
−1
. The electron transfer from Ru metalloligands to Eu(III)
2
catalytic centers are studied via transient absorption and theoretical calculations, shedding light on the photocatalytic mechanism. This work highlights opportunities in photo-generation of highly active lanthanide clusters stabilized in MOFs, which not only enables efficient photocatalysis but also facilitates mechanistic investigation of photo-driven charge separation processes.
Solar-to-chemical CO
2
reduction provides a means to use light’s energy for CO
2
removal and upgrading to useful products, although this photochemical conversion is challenging. Here, authors construct a Europium-containing metal-organic framework that selectively converts CO
2
to formate with light.
Publisher
Nature Publishing Group UK
