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.

Dinuclear uranium(vi) salen coordination compound: An efficient visible-light-active catalyst for selective reduction of CO2to methanol / Azam, M.; Kumar, U.; Olowoyo, J. O.; Al-Resayes, S. I.; Trzesowska-Kruszynska, A.; Kruszynski, R.; Islam, M. S.; Khan, M. R.; Adil, S. F.; Siddiqui, M. R.; Al-Harthi, F. A.; Alinzi, A. K.; Wabaidur, S. M.; Siddiqui, M. R.; Shaik, M. R.; Jain, S. L.; Farkhondehfal, M. Amin.; HERNANDEZ RIBULLEN, SIMELYS PRIS. - In: DALTON TRANSACTIONS. - ISSN 1477-9226. - ELETTRONICO. - 49:47(2020), pp. 17243-17251. [10.1039/d0dt02620d]

Dinuclear uranium(vi) salen coordination compound: An efficient visible-light-active catalyst for selective reduction of CO2to methanol

Farkhondehfal M. Amin.;Hernandez Ribullen Simelys Pris
2020

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.
2020
File in questo prodotto:
File Dimensione Formato  
Dinuclear U(VI) salen coordination compound - vis-light-active PC x methanol prod (M Azam'20).pdf

accesso riservato

Descrizione: Versione finale del editore
Tipologia: 2a Post-print versione editoriale / Version of Record
Licenza: Non Pubblico - Accesso privato/ristretto
Dimensione 2.37 MB
Formato Adobe PDF
2.37 MB Adobe PDF   Visualizza/Apri   Richiedi una copia
Pubblicazioni consigliate

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11583/2954235