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Electrocatalytic water oxidation by a molecular catalyst incorporated into a metal-organic framework thin film
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
2017 (English)In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 46, no 5, 1382-1388 p.Article in journal (Refereed) Published
Abstract [en]

A molecular water oxidation catalyst, [Ru(tpy)(dcbpy)(OH2)](ClO4)(2) (tpy = 2,2': 6',2''-terpyridine, dcbpy = 2,2'-bipyridine- 5,5'-dicarboxylic acid) [1], has been incorporated into FTO-grown thin films of UiO-67 (UiO = University of Oslo), by post-synthetic ligand exchange. Cyclic voltammograms (0.1 M borate buffer at pH = 8.4) of the resulting UiO67-[RuOH2]@ FTO show a reversible wave associated with the Ru-III/II couple in the anodic scan, followed by a large current response that arises from electrocatalytic water oxidation beyond 1.1 V vs. Ag/AgCl. Water oxidation can be observed at an applied potential of 1.5 V over the timescale of hours with a current density of 11.5 mu A cm(-2). Oxygen evolution was quantified in situ over the course of the experiment, and the Faradaic efficiency was calculated as 82%. Importantly, the molecular integrity of [1] during electrocatalytic water oxidation is maintained even on the timescale of hours under turnover conditions and applied voltage, as evidenced by the persistence of the wave associated with the Ru-III/II couple in the CV. This experiment highlights the capability of metal organic frameworks like UiO-67 to stabilize the molecular structure of catalysts that are prone to form higher clusters in homogenous phase.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2017. Vol. 46, no 5, 1382-1388 p.
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-319681DOI: 10.1039/c6dt03718frsc.li/daltonISI: 000395442700005PubMedID: 27845800OAI: oai:DiVA.org:uu-319681DiVA: diva2:1087437
Funder
Swedish Research CouncilSwedish Energy AgencyKnut and Alice Wallenberg Foundation
Available from: 2017-04-07 Created: 2017-04-07 Last updated: 2017-04-07Bibliographically approved

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