Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework

Martino Rimoldi, Leighanne C. Gallington, Karena W. Chapman, Keith William Macrenaris, Joseph T Hupp, Omar k Farha*

*Corresponding author for this work

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

Post-synthetic modification of the zirconium-based metal–organic framework (MOF) NU-1000 by atomic layer deposition (ALD), using tetramethoxysilane (Si(OMe)4) as a precursor, led to the incorporation and stabilization of silicon oxide clusters composed of only a few silicon atoms in the framework's pores. The resulting SiOx functionalized material (Si-NU-1000) was found to be catalytically active despite the inactivity of related bulk silicon dioxide (SiO2), thus demonstrating the positive effects of having nanosized clusters of SiOx. Moreover, Si-NU-1000 showed activity greater than that found for aluminum oxide based catalysts—oxides known for their high acidity—such as an aluminum oxide functionalized MOF (Al-NU-1000) and bulk γ-Al2O3. X-ray photoelectron spectroscopy and infrared spectroscopy measurements unmasked the electron donating nature of Si-NU-1000, explaining the unusual electronic properties of the nanosized SiOx clusters and supporting their high catalytic activity.

Original languageEnglish (US)
Pages (from-to)8532-8536
Number of pages5
JournalChemistry - A European Journal
Volume23
Issue number35
DOIs
StatePublished - Jun 22 2017

Fingerprint

Aluminum Oxide
Nanoclusters
Silicon oxides
Aluminum
Oxides
Atomic layer deposition
Silicon
Zirconium
Silicon Dioxide
Electronic properties
Infrared spectroscopy
Catalyst activity
X ray photoelectron spectroscopy
Stabilization
Silica
Atoms
Electrons
tetramethoxysilane

Keywords

  • atomic layer deposition
  • gas flow catalysis
  • metal–organic frameworks
  • nanocluster
  • silicon oxide

ASJC Scopus subject areas

  • Catalysis
  • Organic Chemistry

Cite this

Rimoldi, Martino ; Gallington, Leighanne C. ; Chapman, Karena W. ; Macrenaris, Keith William ; Hupp, Joseph T ; Farha, Omar k. / Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework. In: Chemistry - A European Journal. 2017 ; Vol. 23, No. 35. pp. 8532-8536.
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Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework. / Rimoldi, Martino; Gallington, Leighanne C.; Chapman, Karena W.; Macrenaris, Keith William; Hupp, Joseph T; Farha, Omar k.

In: Chemistry - A European Journal, Vol. 23, No. 35, 22.06.2017, p. 8532-8536.

Research output: Contribution to journalArticle

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T1 - Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework

AU - Rimoldi, Martino

AU - Gallington, Leighanne C.

AU - Chapman, Karena W.

AU - Macrenaris, Keith William

AU - Hupp, Joseph T

AU - Farha, Omar k

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Y1 - 2017/6/22

N2 - Post-synthetic modification of the zirconium-based metal–organic framework (MOF) NU-1000 by atomic layer deposition (ALD), using tetramethoxysilane (Si(OMe)4) as a precursor, led to the incorporation and stabilization of silicon oxide clusters composed of only a few silicon atoms in the framework's pores. The resulting SiOx functionalized material (Si-NU-1000) was found to be catalytically active despite the inactivity of related bulk silicon dioxide (SiO2), thus demonstrating the positive effects of having nanosized clusters of SiOx. Moreover, Si-NU-1000 showed activity greater than that found for aluminum oxide based catalysts—oxides known for their high acidity—such as an aluminum oxide functionalized MOF (Al-NU-1000) and bulk γ-Al2O3. X-ray photoelectron spectroscopy and infrared spectroscopy measurements unmasked the electron donating nature of Si-NU-1000, explaining the unusual electronic properties of the nanosized SiOx clusters and supporting their high catalytic activity.

AB - Post-synthetic modification of the zirconium-based metal–organic framework (MOF) NU-1000 by atomic layer deposition (ALD), using tetramethoxysilane (Si(OMe)4) as a precursor, led to the incorporation and stabilization of silicon oxide clusters composed of only a few silicon atoms in the framework's pores. The resulting SiOx functionalized material (Si-NU-1000) was found to be catalytically active despite the inactivity of related bulk silicon dioxide (SiO2), thus demonstrating the positive effects of having nanosized clusters of SiOx. Moreover, Si-NU-1000 showed activity greater than that found for aluminum oxide based catalysts—oxides known for their high acidity—such as an aluminum oxide functionalized MOF (Al-NU-1000) and bulk γ-Al2O3. X-ray photoelectron spectroscopy and infrared spectroscopy measurements unmasked the electron donating nature of Si-NU-1000, explaining the unusual electronic properties of the nanosized SiOx clusters and supporting their high catalytic activity.

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