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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

Lookup NU author(s): Dr Joshua Karlsson, Professor Elizabeth GibsonORCiD

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This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).

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.

Publication metadata

Author(s): Cerpentier FJR, Karlsson J, Lalrempui R, Brandon MP, Sazanovich IV, Greetham GM, Gibson EA, Pryce MT

Publication type: Article

Publication status: Published

Journal: Frontiers in Chemistry

Year: 2021

Volume: 9

Online publication date: 24/12/2021

Acceptance date: 29/11/2021

Date deposited: 10/01/2022

ISSN (electronic): 2296-2646

Publisher: Frontiers Research Foundation

URL: https://doi.org/10.3389/fchem.2021.795877

DOI: 10.3389/fchem.2021.795877

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Funding

Funder referenceFunder name
JK and EG also thank Newcastle University and The North East Centre for Energy Materials (EP/R021503/1) for funding.
Project 785 “HYLANTIC” (EAPA_204/2016), which is co-financed by 786 the European Regional Development Found in the framework 787 of the Interreg Atlantic programme.
Sustainable Energy Authority of Ireland under the SEAI National Energy Research, Development and Demonstration Funding Programme 2018 and 2019, Grant numbers 18/RDD/282 and 19/RDD/566

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