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

7 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)201-212
Number of pages12
JournalFaraday Discussions
Volume201
DOIs
Publication statusPublished - Jan 1 2017

Fingerprint

Iridium
Atomic layer deposition
atomic layer epitaxy
iridium
Aluminum
Catalyst supports
Tuning
Metals
tuning
Ions
Carbon Monoxide
aluminum
catalysts
Catalysts
ethylene
metals
ions
Dimerization
Steam
dimerization

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Tuning the properties of metal-organic framework nodes as supports of single-site iridium catalysts : Node modification by atomic layer deposition of aluminium. / Yang, Dong; Momeni, Mohammad R.; Demir, Hakan; Pahls, Dale R.; Rimoldi, Martino; Wang, Timothy C.; Farha, Omar K.; Hupp, Joseph T; Cramer, Christopher J.; Gates, Bruce C.; Gagliardi, Laura.

In: Faraday Discussions, Vol. 201, 01.01.2017, p. 201-212.

Research output: Contribution to journalReview article

Yang, Dong ; Momeni, Mohammad R. ; Demir, Hakan ; Pahls, Dale R. ; Rimoldi, Martino ; Wang, Timothy C. ; Farha, Omar K. ; Hupp, Joseph T ; Cramer, Christopher J. ; Gates, Bruce C. ; Gagliardi, Laura. / Tuning the properties of metal-organic framework nodes as supports of single-site iridium catalysts : Node modification by atomic layer deposition of aluminium. In: Faraday Discussions. 2017 ; Vol. 201. pp. 201-212.
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AU - Wang, Timothy C.

AU - Farha, Omar K.

AU - Hupp, Joseph T

AU - Cramer, Christopher J.

AU - Gates, Bruce C.

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