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Issue 5, 2017
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Electrocatalytic water oxidation by a molecular catalyst incorporated into a metal–organic framework thin film

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Abstract

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 RuIII/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 μA 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 RuIII/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.

Graphical abstract: Electrocatalytic water oxidation by a molecular catalyst incorporated into a metal–organic framework thin film

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Publication details

The article was received on 24 Sep 2016, accepted on 01 Nov 2016 and first published on 08 Nov 2016


Article type: Paper
DOI: 10.1039/C6DT03718F
Dalton Trans., 2017,46, 1382-1388

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    Electrocatalytic water oxidation by a molecular catalyst incorporated into a metal–organic framework thin film

    B. A. Johnson, A. Bhunia and S. Ott, Dalton Trans., 2017, 46, 1382
    DOI: 10.1039/C6DT03718F

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