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Volume 201, 2017
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Tuning the properties of metal–organic framework nodes as supports of single-site iridium catalysts: node modification by atomic layer deposition of aluminium

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Abstract

The metal–organic framework NU-1000, with Zr6-oxo, hydroxo, and aqua nodes, was modified by incorporation of hydroxylated Al(III) ions by ALD-like chemistry with [Al(CH3)2(iso-propoxide)]2 followed by steam (ALD = atomic layer deposition). Al ions were installed to the extent of approximately 7 per node. Single-site iridium diethylene complexes were anchored to the nodes of the modified and unmodified MOFs by reaction with Ir(C2H4)2(acac) (acac = acetylacetonate) and converted to Ir(CO)2 complexes by treatment with CO. Infrared spectra of these supported complexes show that incorporation of Al weakened the electron donor tendency of the MOF. Correspondingly, the catalytic activity of the initial supported iridium complexes for ethylene hydrogenation increased, as did the selectivity for ethylene dimerization. The results of density functional theory calculations with a simplified model of the nodes incorporating Al(III) ions are in qualitative agreement with some catalyst performance data.

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Publication details

The article was received on 22 Jan 2017, accepted on 20 Feb 2017 and first published on 20 Feb 2017


Article type: Paper
DOI: 10.1039/C7FD00031F
Citation: Faraday Discuss., 2017,201, 195-206
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    Tuning the properties of metal–organic framework nodes as supports of single-site iridium catalysts: node modification by atomic layer deposition of aluminium

    D. Yang, M. R. Momeni, H. Demir, D. R. Pahls, M. Rimoldi, T. C. Wang, O. K. Farha, J. T. Hupp, C. J. Cramer, B. C. Gates and L. Gagliardi, Faraday Discuss., 2017, 201, 195
    DOI: 10.1039/C7FD00031F

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