skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Pore-Templated Growth of Catalytically Active Gold Nanoparticles within a Metal–Organic Framework

Abstract

Obtaining persistently well-dispersed gold nano-particles (AuNPs) on solid support with optimum particle size for heterogeneous catalysis can be challenging. Here, we report on the channel-templated growth of AuNPs within a stable zirconium-based metal–organic framework, NU-1000, via channel-anchored monometallic precursors. Pair distribution function analysis of total X-ray scattering by the incorporated face-centered-cubic nanopar-ticles reveals a bimodal size distribution, with ca. 98% of the en-shrouded nanoparticles having a diameter that closely reflects the ~10 Å width of triangular pores and with ca. 2% closely reflecting the ~31 Å width of hexagonal pores of NU-1000. The resulting ma-terial is catalytically active (and recyclable) for condensed-phase hydrogenation of 4-nitrophenol to 4-aminophenol.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4];  [1]; ORCiD logo [5]; ORCiD logo [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Northwestern Univ., Evanston, IL (United States); Kyoto Univ., Kyoto (Japan)
  4. Northwestern Univ., Evanston, IL (United States); National Cheng Kung Univ., Tainan City (Taiwan)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); Stony Brook Univ., Stony Brook, NY (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)
OSTI Identifier:
1524086
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 5; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Goswami, Subhadip, Noh, Hyunho, Redfern, Louis R., Otake, Ken-ichi, Kung, Chung -Wei, Cui, Yuexing, Chapman, Karena W., Farha, Omar K., and Hupp, Joseph T.. Pore-Templated Growth of Catalytically Active Gold Nanoparticles within a Metal–Organic Framework. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.chemmater.8b04983.
Goswami, Subhadip, Noh, Hyunho, Redfern, Louis R., Otake, Ken-ichi, Kung, Chung -Wei, Cui, Yuexing, Chapman, Karena W., Farha, Omar K., & Hupp, Joseph T.. Pore-Templated Growth of Catalytically Active Gold Nanoparticles within a Metal–Organic Framework. United States. https://doi.org/10.1021/acs.chemmater.8b04983
Goswami, Subhadip, Noh, Hyunho, Redfern, Louis R., Otake, Ken-ichi, Kung, Chung -Wei, Cui, Yuexing, Chapman, Karena W., Farha, Omar K., and Hupp, Joseph T.. Mon . "Pore-Templated Growth of Catalytically Active Gold Nanoparticles within a Metal–Organic Framework". United States. https://doi.org/10.1021/acs.chemmater.8b04983. https://www.osti.gov/servlets/purl/1524086.
@article{osti_1524086,
title = {Pore-Templated Growth of Catalytically Active Gold Nanoparticles within a Metal–Organic Framework},
author = {Goswami, Subhadip and Noh, Hyunho and Redfern, Louis R. and Otake, Ken-ichi and Kung, Chung -Wei and Cui, Yuexing and Chapman, Karena W. and Farha, Omar K. and Hupp, Joseph T.},
abstractNote = {Obtaining persistently well-dispersed gold nano-particles (AuNPs) on solid support with optimum particle size for heterogeneous catalysis can be challenging. Here, we report on the channel-templated growth of AuNPs within a stable zirconium-based metal–organic framework, NU-1000, via channel-anchored monometallic precursors. Pair distribution function analysis of total X-ray scattering by the incorporated face-centered-cubic nanopar-ticles reveals a bimodal size distribution, with ca. 98% of the en-shrouded nanoparticles having a diameter that closely reflects the ~10 Å width of triangular pores and with ca. 2% closely reflecting the ~31 Å width of hexagonal pores of NU-1000. The resulting ma-terial is catalytically active (and recyclable) for condensed-phase hydrogenation of 4-nitrophenol to 4-aminophenol.},
doi = {10.1021/acs.chemmater.8b04983},
journal = {Chemistry of Materials},
number = 5,
volume = 31,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Surface plasmon subwavelength optics
journal, August 2003

  • Barnes, William L.; Dereux, Alain; Ebbesen, Thomas W.
  • Nature, Vol. 424, Issue 6950, p. 824-830
  • DOI: 10.1038/nature01937

Unraveling the Effects of Size, Composition, and Substrate on the Localized Surface Plasmon Resonance Frequencies of Gold and Silver Nanocubes: A Systematic Single-Particle Approach
journal, June 2010

  • Ringe, Emilie; McMahon, Jeffrey M.; Sohn, Kwonnam
  • The Journal of Physical Chemistry C, Vol. 114, Issue 29
  • DOI: 10.1021/jp104366r

Controlled Plasmonic Nanostructures for Surface-Enhanced Spectroscopy and Sensing
journal, December 2008

  • Camden, Jon P.; Dieringer, Jon A.; Zhao, Jing
  • Accounts of Chemical Research, Vol. 41, Issue 12
  • DOI: 10.1021/ar800041s

The Optical Properties of Metal Nanoparticles:  The Influence of Size, Shape, and Dielectric Environment
journal, January 2003

  • Kelly, K. Lance; Coronado, Eduardo; Zhao, Lin Lin
  • The Journal of Physical Chemistry B, Vol. 107, Issue 3
  • DOI: 10.1021/jp026731y

Self-Assembled Plasmonic Nanoparticle Clusters
journal, May 2010


Gold Nanoparticle-Based Sensing of “Spectroscopically Silent” Heavy Metal Ions
journal, April 2001

  • Kim, Youngjin; Johnson, Robert C.; Hupp, Joseph T.
  • Nano Letters, Vol. 1, Issue 4
  • DOI: 10.1021/nl0100116

A DNA-based method for rationally assembling nanoparticles into macroscopic materials
journal, August 1996

  • Mirkin, Chad A.; Letsinger, Robert L.; Mucic, Robert C.
  • Nature, Vol. 382, Issue 6592, p. 607-609
  • DOI: 10.1038/382607a0

Gold nanoparticles: preparation, properties, and applications in bionanotechnology
journal, January 2012

  • Yeh, Yi-Cheun; Creran, Brian; Rotello, Vincent M.
  • Nanoscale, Vol. 4, Issue 6
  • DOI: 10.1039/C1NR11188D

When Gold Is Not Noble: Catalysis by Nanoparticles
journal, April 2003


Catalysis and Photocatalysis by Nanoscale Au/TiO 2 : Perspectives for Renewable Energy
journal, April 2017


Activation of Oxygen on Gold/Alumina Catalysts: In Situ High-Energy-Resolution Fluorescence and Time-Resolved X-ray Spectroscopy
journal, July 2006

  • van Bokhoven, Jeroen A.; Louis, Catherine; Miller, Jeffrey T.
  • Angewandte Chemie International Edition, Vol. 45, Issue 28
  • DOI: 10.1002/anie.200601184

Special Sites at Noble and Late Transition Metal Catalysts
journal, March 2006


High-Temperature Stable Gold Nanoparticle Catalysts for Application under Severe Conditions: The Role of TiO 2 Nanodomains in Structure and Activity
journal, January 2015

  • Puértolas, Begoña; Mayoral, Álvaro; Arenal, Raul
  • ACS Catalysis, Vol. 5, Issue 2
  • DOI: 10.1021/cs501741u

Spectroscopic Evidence for the Supply of Reactive Oxygen during CO Oxidation Catalyzed by Gold Supported on Nanocrystalline CeO 2
journal, March 2005

  • Guzman, Javier; Carrettin, Silvio; Corma, Avelino
  • Journal of the American Chemical Society, Vol. 127, Issue 10
  • DOI: 10.1021/ja043752s

A Nanoreactor Framework of a Au@SiO2 Yolk/Shell Structure for Catalytic Reduction ofp-Nitrophenol
journal, April 2008

  • Lee, Joongoo; Park, Ji Chan; Song, Hyunjoon
  • Advanced Materials, Vol. 20, Issue 8
  • DOI: 10.1002/adma.200702338

Size- and support-dependency in the catalysis of gold
journal, April 1997


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

  • Mondloch, Joseph E.; Bury, Wojciech; Fairen-Jimenez, David
  • Journal of the American Chemical Society, Vol. 135, Issue 28, p. 10294-10297
  • DOI: 10.1021/ja4050828

Scalable synthesis and post-modification of a mesoporous metal-organic framework called NU-1000
journal, December 2015

  • Wang, Timothy C.; Vermeulen, Nicolaas A.; Kim, In Soo
  • Nature Protocols, Vol. 11, Issue 1
  • DOI: 10.1038/nprot.2016.001

Deposition of Gold Clusters on Porous Coordination Polymers by Solid Grinding and Their Catalytic Activity in Aerobic Oxidation of Alcohols
journal, September 2008

  • Ishida, Tamao; Nagaoka, Megumi; Akita, Tomoki
  • Chemistry - A European Journal, Vol. 14, Issue 28
  • DOI: 10.1002/chem.200800980

Au@ZIFs: Stabilization and Encapsulation of Cavity-Size Matching Gold Clusters inside Functionalized Zeolite Imidazolate Frameworks, ZIFs
journal, December 2010

  • Esken, Daniel; Turner, Stuart; Lebedev, Oleg I.
  • Chemistry of Materials, Vol. 22, Issue 23
  • DOI: 10.1021/cm102529c

A smart approach to achieve an exceptionally high loading of metal nanoparticles supported by functionalized extended frameworks for efficient catalysis
journal, January 2015

  • Gole, Bappaditya; Sanyal, Udishnu; Mukherjee, Partha Sarathi
  • Chemical Communications, Vol. 51, Issue 23
  • DOI: 10.1039/C4CC09228G

Metal@MOF: Loading of Highly Porous Coordination Polymers Host Lattices by Metal Organic Chemical Vapor Deposition
journal, September 2005

  • Hermes, Stephan; Schröter, Marie-Katrin; Schmid, Rochus
  • Angewandte Chemie International Edition, Vol. 44, Issue 38, p. 6237-6241
  • DOI: 10.1002/anie.200462515

Copper Nanocrystals Encapsulated in Zr-based Metal–Organic Frameworks for Highly Selective CO 2 Hydrogenation to Methanol
journal, November 2016


Addressing the characterisation challenge to understand catalysis in MOFs: the case of nanoscale Cu supported in NU-1000
journal, January 2017

  • Platero-Prats, Ana E.; Li, Zhanyong; Gallington, Leighanne C.
  • Faraday Discussions, Vol. 201
  • DOI: 10.1039/C7FD00110J

Metal-Organic Framework Templated Synthesis of Ultrathin, Well-Aligned Metallic Nanowires
journal, February 2015

  • Volosskiy, Boris; Niwa, Kenta; Chen, Yu
  • ACS Nano, Vol. 9, Issue 3
  • DOI: 10.1021/nn5072446

Controlled synthesis of novel Au@MIL-100(Fe) core–shell nanoparticles with enhanced catalytic performance
journal, January 2013

  • Ke, Fei; Zhu, Junfa; Qiu, Ling-Guang
  • Chem. Commun., Vol. 49, Issue 13
  • DOI: 10.1039/C2CC33964A

Imparting functionality to a metal–organic framework material by controlled nanoparticle encapsulation
journal, February 2012

  • Lu, Guang; Li, Shaozhou; Guo, Zhen
  • Nature Chemistry, Vol. 4, Issue 4, p. 310-316
  • DOI: 10.1038/nchem.1272

Confinement of Ultrasmall Cu/ZnO x Nanoparticles in Metal–Organic Frameworks for Selective Methanol Synthesis from Catalytic Hydrogenation of CO 2
journal, March 2017

  • An, Bing; Zhang, Jingzheng; Cheng, Kang
  • Journal of the American Chemical Society, Vol. 139, Issue 10
  • DOI: 10.1021/jacs.7b00058

Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework
journal, January 2018

  • Kim, In Soo; Li, Zhanyong; Zheng, Jian
  • Angewandte Chemie International Edition, Vol. 57, Issue 4
  • DOI: 10.1002/anie.201708092

Metal–Organic Frameworks Containing (Alkynyl)Gold Functionalities: A Comparative Evaluation of Solvent-Assisted Linker Exchange, de Novo Synthesis, and Post-synthesis Modification
journal, October 2014

  • Madrahimov, Sherzod T.; Atesin, Tulay A.; Karagiaridi, Olga
  • Crystal Growth & Design, Vol. 14, Issue 12
  • DOI: 10.1021/cg501066s

Chemical, thermal and mechanical stabilities of metal–organic frameworks
journal, February 2016


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

  • Bai, Yan; Dou, Yibo; Xie, Lin-Hua
  • Chemical Society Reviews, Vol. 45, Issue 8
  • DOI: 10.1039/C5CS00837A

Zr(iv) and Hf(iv) based metal–organic frameworks with reo-topology
journal, January 2012

  • Bon, Volodymyr; Senkovskyy, Volodymyr; Senkovska, Irena
  • Chemical Communications, Vol. 48, Issue 67
  • DOI: 10.1039/c2cc34246d

A New Zirconium Inorganic Building Brick Forming Metal Organic Frameworks with Exceptional Stability
journal, October 2008

  • Cavka, Jasmina Hafizovic; Jakobsen, Søren; Olsbye, Unni
  • Journal of the American Chemical Society, Vol. 130, Issue 42, p. 13850-13851
  • DOI: 10.1021/ja8057953

Versatile functionalization of the NU-1000 platform by solvent-assisted ligand incorporation
journal, January 2014

  • Deria, Pravas; Bury, Wojciech; Hupp, Joseph T.
  • Chemical Communications, Vol. 50, Issue 16, p. 1965-1968
  • DOI: 10.1039/c3cc48562e

Copper Nanoparticles Installed in Metal–Organic Framework Thin Films are Electrocatalytically Competent for CO 2 Reduction
journal, September 2017


FTIR Study of CO Oxidation on Au/TiO 2 at 90 K and Room Temperature. An Insight into the Nature of the Reaction Centers
journal, June 2000

  • Boccuzzi, Flora; Chiorino, Anna
  • The Journal of Physical Chemistry B, Vol. 104, Issue 23
  • DOI: 10.1021/jp000749w

A porous, electrically conductive hexa-zirconium( iv ) metal–organic framework
journal, January 2018

  • Goswami, Subhadip; Ray, Debmalya; Otake, Ken-ichi
  • Chemical Science, Vol. 9, Issue 19
  • DOI: 10.1039/C8SC00961A

Nitroarene reduction: a trusted model reaction to test nanoparticle catalysts
journal, January 2015

  • Aditya, Teresa; Pal, Anjali; Pal, Tarasankar
  • Chemical Communications, Vol. 51, Issue 46, p. 9410-9431
  • DOI: 10.1039/C5CC01131K

The critical role of water at the gold-titania interface in catalytic CO oxidation
journal, September 2014


    Works referencing / citing this record:

    Controlled Growth of Ag Nanocrystals in a H‐Bonded Open Framework
    journal, September 2019

    • Khodja, Walid; Collière, Vincent; Kahn, Myrtil L.
    • Chemistry – A European Journal, Vol. 25, Issue 60
    • DOI: 10.1002/chem.201903684

    Nanofabrication of Au nanoparticles over conductive metallohydrogel nanofibers for nanocatalysis application
    journal, January 2020

    • Dixit, Manish Kumar; Chery, Déborah; Mahendar, Chinthakuntla
    • Inorganic Chemistry Frontiers, Vol. 7, Issue 4
    • DOI: 10.1039/c9qi01514k