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

Rimoldi, Martino; Gallington, Leighanne C.; Chapman, Karena W.; MacRenaris, Keith; Hupp, Joseph T.; Farha, Omar K.

doi:10.1002/chem.201701902

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

Abstract

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 SiO _x functionalized material (Si‐NU‐1000) was found to be catalytically active despite the inactivity of related bulk silicon dioxide (SiO ₂ ), thus demonstrating the positive effects of having nanosized clusters of SiO _x . 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‐Al ₂ O ₃ . 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 SiO _x clusters and supporting their high catalytic activity.

Authors:

^[1]; Gallington, Leighanne C. ^[2]; Chapman, Karena W. ^[2]; MacRenaris, Keith ^[1]; Hupp, Joseph T. ^[1]; Farha, Omar K. ^[3]

Department of Chemistry Northwestern University 2145 Sheridan Road Evanston Illinois 60208 USA
X-ray Science Division Advanced Photon Source Argonne National Laboratory 9700 S. Cass Avenue Argonne Illinois 60439 USA
Department of Chemistry Northwestern University 2145 Sheridan Road Evanston Illinois 60208 USA, Department of Chemistry Faculty of Science King Abdulaziz University Jeddah 21589 Saudi Arabia

Publication Date:: Tue May 30 00:00:00 EDT 2017

Sponsoring Org.:: USDOE

OSTI Identifier:: 1401064

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Chemistry - A European Journal

Additional Journal Information:: Journal Name: Chemistry - A European Journal Journal Volume: 23 Journal Issue: 35; Journal ID: ISSN 0947-6539

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Rimoldi, Martino, Gallington, Leighanne C., Chapman, Karena W., MacRenaris, Keith, Hupp, Joseph T., and Farha, Omar K. Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework.  Germany: N. p., 2017. 
Web.  doi:10.1002/chem.201701902.

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                    Rimoldi, Martino, Gallington, Leighanne C., Chapman, Karena W., MacRenaris, Keith, Hupp, Joseph T., & Farha, Omar K. Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework.  Germany.  https://doi.org/10.1002/chem.201701902

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                    Rimoldi, Martino, Gallington, Leighanne C., Chapman, Karena W., MacRenaris, Keith, Hupp, Joseph T., and Farha, Omar K. Tue .  
"Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework".  Germany.  https://doi.org/10.1002/chem.201701902.

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@article{osti_1401064,

  title        = {Catalytically Active Silicon Oxide Nanoclusters Stabilized in a Metal–Organic Framework},

  author       = {Rimoldi, Martino and Gallington, Leighanne C. and Chapman, Karena W. and MacRenaris, Keith and Hupp, Joseph T. and Farha, Omar K.},

  abstractNote = {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 SiO x functionalized material (Si‐NU‐1000) was found to be catalytically active despite the inactivity of related bulk silicon dioxide (SiO 2 ), thus demonstrating the positive effects of having nanosized clusters of SiO x . 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‐Al 2 O 3 . 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 SiO x clusters and supporting their high catalytic activity.},

  doi          = {10.1002/chem.201701902},

  journal      = {Chemistry - A European Journal},

  number       = 35,

  volume       = 23,

  place        = {Germany},

  year         = {Tue May 30 00:00:00 EDT 2017},

  month        = {Tue May 30 00:00:00 EDT 2017}

}

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

Abstract

Citation Formats

Synthesis Modulation as a Tool To Increase the Catalytic Activity of Metal–Organic Frameworks: The Unique Case of UiO-66(Zr) journal, July 2013

Tailoring nanoporous materials by atomic layer deposition journal, January 2011

Atomic Layer Deposition of Pt Nanoparticles within the Cages of MIL-101: A Mild and Recyclable Hydrogenation Catalyst journal, March 2016

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In Situ Reaction Mechanism Studies on Atomic Layer Deposition of Al x Si y O z from Trimethylaluminium, Hexakis(ethylamino)disilane, and Water journal, October 2012

Zr-based metal–organic frameworks: design, synthesis, structure, and applications journal, January 2016

State of the art and future challenges of zeolites as catalysts journal, May 2003

Catalytic Zirconium/Hafnium-Based Metal–Organic Frameworks journal, December 2016

Tuning Acid–Base Properties Using Mg–Al Oxide Atomic Layer Deposition journal, July 2015

Metal–organic framework materials as catalysts journal, January 2009

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Superacidity in Sulfated Metal–Organic Framework-808 journal, September 2014

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Growth of SiO2 at Room Temperature with the Use of Catalyzed Sequential Half-Reactions journal, December 1997

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ALD of SiO[sub 2] at Room Temperature Using TEOS and H[sub 2]O with NH[sub 3] as the Catalyst journal, January 2004

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Inorganic Solid Acids and Their Use in Acid-Catalyzed Hydrocarbon Reactions journal, May 1995

Destruction of chemical warfare agents using metal–organic frameworks journal, March 2015

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Targeted Single-Site MOF Node Modification: Trivalent Metal Loading via Atomic Layer Deposition journal, June 2015

X-Ray photoelectron spectroscopy on zeolites and related materials journal, July 1996

Conformal Coating on Ultrahigh-Aspect-Ratio Nanopores of Anodic Alumina by Atomic Layer Deposition journal, September 2003

Vapor-Phase Metalation by Atomic Layer Deposition in a Metal–Organic Framework journal, May 2013

Brønsted Acidity in Metal–Organic Frameworks journal, June 2015

Towards a molecular understanding of shape selectivity journal, February 2008

Aluminium atomic layer deposition applied to mesoporous zeolites for acid catalytic activity enhancement journal, January 2011

The nature of the relative bonding chemistry in zeolites: An XPS study journal, November 1990

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Growth of SiO2 at Room Temperature with the Use of Catalyzed Sequential Half-Reactions
journal, December 1997

Catalyst Design with Atomic Layer Deposition
journal, February 2015

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journal, April 2009

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journal, January 2017

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journal, November 2013

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journal, January 2010

Electronic Effects of Linker Substitution on Lewis Acid Catalysis with Metal-Organic Frameworks
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Targeted Single-Site MOF Node Modification: Trivalent Metal Loading via Atomic Layer Deposition
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X-Ray photoelectron spectroscopy on zeolites and related materials
journal, July 1996

Conformal Coating on Ultrahigh-Aspect-Ratio Nanopores of Anodic Alumina by Atomic Layer Deposition
journal, September 2003

Vapor-Phase Metalation by Atomic Layer Deposition in a Metal–Organic Framework
journal, May 2013

Brønsted Acidity in Metal–Organic Frameworks
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Towards a molecular understanding of shape selectivity
journal, February 2008

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