Photo-generated dinuclear {Eu(II)}2 active sites for selective CO2 reduction in a photosensitizing metal-organic framework

Zhi-Hao Yan, Ming-Hao Du, Junxue Liu, Shengye Jin, Cheng Wang, Gui-Lin Zhuang, Xiang-Jian Kong (), La-Sheng Long and Lan-Sun Zheng
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Zhi-Hao Yan: Xiamen University
Ming-Hao Du: Xiamen University
Junxue Liu: Chinese Academy of Sciences
Shengye Jin: Chinese Academy of Sciences
Cheng Wang: Xiamen University
Gui-Lin Zhuang: Zhejiang University of Technology
Xiang-Jian Kong: Xiamen University
La-Sheng Long: Xiamen University
Lan-Sun Zheng: Xiamen University

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract Photocatalytic reduction of CO2 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 CO2 reduction. Photo-excitation of the metalloligands initiates electron injection into the nodes to generate dinuclear {Eu(II)}2 active sites, which can selectively reduce CO2 to formate in a two-electron process with a remarkable rate of 321.9 μmol h−1 mmolMOF−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.

Date: 2018
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DOI: 10.1038/s41467-018-05659-7

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