Volume 201, 2017

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

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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Article information

Article type
Paper
Submitted
22 jan 2017
Accepted
20 feb 2017
First published
20 feb 2017

Faraday Discuss., 2017,201, 195-206

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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