Issue 47, 2020

Dinuclear uranium(vi) salen coordination compound: an efficient visible-light-active catalyst for selective reduction of CO2 to methanol

Abstract

A new dinuclear uranyl salen coordination compound, [(UO2)2(L)2]·2MeCN [L = 6,6′-((1E,1′E)-((2,2-dimethylpropane-1,3-diyl)bis(azaneylylidene))-bis(methaneylylidene))bis(2-methoxyphenol)], was synthesized using a multifunctional salen ligand to harvest visible light for the selective photocatalytic reduction of CO2 to MeOH. The assembling of the two U centers into one coordination moiety via a chelating–bridging doubly deprotonated tetradentate ligand allowed the formation of U centers with distorted pentagonal bipyramid geometry. Such construction of compounds leads to excellent activity for the photocatalytic reduction of CO2, permitting a production rate of 1.29 mmol g−1 h−1 of MeOH with an apparent quantum yield of 18%. Triethanolamine (TEOA) was used as a sacrificial electron donor to carry out the photocatalytic reduction of CO2. The selective methanol formation was purely a photocatalytic phenomenon and confirmed using isotopically labeled 13CO2 and product analysis by 13C-NMR spectroscopy. The spectroscopic studies also confirmed the interaction of CO2 with the molecule of the title complex. The results of these efforts made it possible to understand the reaction mechanism using ESI–mass spectrometry.

Graphical abstract: Dinuclear uranium(vi) salen coordination compound: an efficient visible-light-active catalyst for selective reduction of CO2 to methanol

Supplementary files

Article information

Article type
Paper
Submitted
24 Jul 2020
Accepted
25 Okt 2020
First published
02 Nov 2020

Dalton Trans., 2020,49, 17243-17251

Dinuclear uranium(VI) salen coordination compound: an efficient visible-light-active catalyst for selective reduction of CO2 to methanol

M. Azam, U. Kumar, J. O. Olowoyo, S. I. Al-Resayes, A. Trzesowska-Kruszynska, R. Kruszynski, M. S. Islam, M. R. Khan, S. F. Adil, M. R. Siddiqui, F. A. Al-Harthi, A. K. Alinzi, S. M. Wabaidur, M. R. Siddiqui, M. R. Shaik, S. L. Jain, M. A. Farkhondehfal and S. Hernàndez, Dalton Trans., 2020, 49, 17243 DOI: 10.1039/D0DT02620D

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