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

Dong Yang, Mohammad R. Momeni, Hakan Demir, Dale R. Pahls, Martino Rimoldi, Timothy C. Wang, Omar K. Farha, Joseph T. Hupp, Christopher J. Cramer, Bruce C. Gates, Laura Gagliardi

Research output: Contribution to journalReview article

12 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)195-206
Number of pages12
JournalFaraday Discussions
Volume201
DOIs
Publication statusPublished - Jan 1 2017

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

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    Yang, D., Momeni, M. R., Demir, H., Pahls, D. R., Rimoldi, M., Wang, T. C., Farha, O. K., Hupp, J. T., Cramer, C. J., Gates, B. C., & Gagliardi, L. (2017). Tuning the properties of metal-organic framework nodes as supports of single-site iridium catalysts: Node modification by atomic layer deposition of aluminium. Faraday Discussions, 201, 195-206. https://doi.org/10.1039/c7fd00031f