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Issue 12, 2019
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Single-site metal–organic framework catalysts for the oxidative coupling of arenes via C–H/C–H activation

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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

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Publication details

The article was received on 10 Dec 2018, accepted on 17 Feb 2019 and first published on 18 Feb 2019


Article type: Edge Article
DOI: 10.1039/C8SC05510F
Chem. Sci., 2019,10, 3616-3622
  • Open access: Creative Commons BY-NC license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    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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