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Ruthenium Assemblies for CO2 Reduction and H2 Generation: Time Resolved Infrared Spectroscopy, Spectroelectrochemistry and a Photocatalysis Study in Solution and on NiO

Authors
  • Cerpentier, Florian J. R.1
  • Karlsson, Joshua2
  • Lalrempuia, Ralte1, 3
  • Brandon, Michael P.1
  • Sazanovich, Igor V.4
  • Greetham, Gregory M.4
  • Gibson, Elizabeth A.2
  • Pryce, Mary T.1
  • 1 School of Chemical Sciences, Dublin City University, Dublin , (Ireland)
  • 2 Energy Materials Laboratory, Department of Chemistry, School of Natural and Environmental Science, Newcastle University, Newcastle upon Tyne , (United Kingdom)
  • 3 Department of Chemistry, School of Physical Sciences, Mizoram University, Aizawl , (India)
  • 4 Central Laser Facility, Science and Technology Facilities Council, Research Complex at Harwell, Rutherford Appleton Laboratory, Oxford , (United Kingdom)
Type
Published Article
Journal
Frontiers in Chemistry
Publisher
Frontiers Media S.A.
Publication Date
Dec 24, 2021
Volume
9
Identifiers
DOI: 10.3389/fchem.2021.795877
Source
Frontiers
Keywords
Disciplines
  • Chemistry
  • Original Research
License
Green

Abstract

Two novel supramolecular complexes RuRe ([Ru(dceb)2(bpt)Re(CO)3Cl](PF6)) and RuPt ([Ru(dceb)2(bpt)PtI(H2O)](PF6)2) [dceb = diethyl(2,2′-bipyridine)-4,4′-dicarboxylate, bpt = 3,5-di(pyridine-2-yl)-1,2,4-triazolate] were synthesized as new catalysts for photocatalytic CO2 reduction and H2 evolution, respectively. The influence of the catalytic metal for successful catalysis in solution and on a NiO semiconductor was examined. IR-active handles in the form of carbonyl groups on the peripheral ligand on the photosensitiser were used to study the excited states populated, as well as the one-electron reduced intermediate species using infrared and UV-Vis spectroelectrochemistry, and time resolved infrared spectroscopy. Inclusion of ethyl-ester moieties led to a reduction in the LUMO energies on the peripheral bipyridine ligand, resulting in localization of the 3MLCT excited state on these peripheral ligands following excitation. RuPt generated hydrogen in solution and when immobilized on NiO in a photoelectrochemical (PEC) cell. RuRe was inactive as a CO2 reduction catalyst in solution, and produced only trace amounts of CO when the photocatalyst was immobilized on NiO in a PEC cell saturated with CO2.

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