Issue 12, 2019

Single-site metal–organic framework catalysts for the oxidative coupling of arenes via C–H/C–H activation

Abstract

C–H activation reactions are generally associated with relatively low turnover numbers (TONs) and high catalyst concentrations due to a combination of low catalyst stability and activity, highlighting the need for recyclable heterogeneous catalysts with stable single-atom active sites. In this work, several palladium loaded metal–organic frameworks (MOFs) were tested as single-site catalysts for the oxidative coupling of arenes (e.g. o-xylene) via C–H/C–H activation. Isolation of the palladium active sites on the MOF supports reduced Pd(0) aggregate formation and thus catalyst deactivation, resulting in higher turnover numbers (TONs) compared to the homogeneous benchmark reaction. Notably, a threefold higher TON could be achieved for palladium loaded MOF-808 due to increased catalyst stability and the heterogeneous catalyst could efficiently be reused, resulting in a cumulative TON of 1218 after three runs. Additionally, the palladium single-atom active sites on MOF-808 were successfully identified by Fourier transform infrared (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy.

Graphical abstract: Single-site metal–organic framework catalysts for the oxidative coupling of arenes via C–H/C–H activation

Supplementary files

Article information

Article type
Edge Article
Submitted
10 Dec. 2018
Accepted
17 Febr. 2019
First published
18 Febr. 2019
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2019,10, 3616-3622

Single-site metal–organic framework catalysts for the oxidative coupling of arenes via C–H/C–H activation

N. Van Velthoven, S. Waitschat, S. M. Chavan, P. Liu, S. Smolders, J. Vercammen, B. Bueken, S. Bals, K. P. Lillerud, N. Stock and D. E. De Vos, Chem. Sci., 2019, 10, 3616 DOI: 10.1039/C8SC05510F

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