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Issue 39, 2020
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Synthetic strategies to incorporate Ru-terpyridyl water oxidation catalysts into MOFs: direct synthesis vs. post-synthetic approach

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Abstract

Incorporating molecular catalysts into metal–organic frameworks (MOFs) is a promising strategy for improving their catalytic longevity and recyclability. In this article, we investigate and compare synthetic routes for the incorporation of the potent water oxidation catalyst Ru(tda)(pyCO2H)2 (tda = 2,2′:6′,2′′-terpyridine-6,6′′-dicarboxylic acid, pyCO2H = iso-nicotinic acid) as a structural linker into a Zr-based UiO-type MOF. The task is challenging with this particular metallo-linker because of the equatorial dangling carboxylates that can potentially compete for Zr-coordination, as well as free rotation of the pyCO2H groups around the HO2Cpy⋯Ru⋯pyCO2H axis. As a consequence, all attempts to synthesize a MOF with the metallo-linker directly under solvothermal conditions led to amorphous materials with the Ru(tda)(pyCO2H)2 linker coordinating to the Zr nodes in ill-defined ways, resulting in multiple waves in the cyclic voltammograms of the solvothermally obtained materials. On the other hand, an indirect post-synthetic approach in which the Ru(tda)(pyCO2H)2 linker is introduced into a preformed edba-MOF (edba = ethyne dibenzoic acid) of UiO topology results in the formation of the desired material. Interestingly, two distinctly different morphologies of the parent edba-MOF have been discovered, and the impact that the morphological difference has on linker incorporation is investigated.

Graphical abstract: Synthetic strategies to incorporate Ru-terpyridyl water oxidation catalysts into MOFs: direct synthesis vs. post-synthetic approach

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Supplementary files

Article information


Submitted
26 May 2020
Accepted
17 Sep 2020
First published
25 Sep 2020

This article is Open Access

Dalton Trans., 2020,49, 13753-13759
Article type
Paper

Synthetic strategies to incorporate Ru-terpyridyl water oxidation catalysts into MOFs: direct synthesis vs. post-synthetic approach

T. Liseev, A. Howe, M. A. Hoque, C. Gimbert-Suriñach, A. Llobet and S. Ott, Dalton Trans., 2020, 49, 13753
DOI: 10.1039/D0DT01890B

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