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

Title: Identification of active sites on supported metal catalysts with carbon nanotube hydrogen highways

Abstract

Catalysts consisting of metal particles supported on reducible oxides exhibit promising activity and selectivity for a variety of current and emerging industrial processes. Enhanced catalytic activity can arise from direct contact between the support and the metal or from metal-induced promoter effects on the oxide. Discovering the source of enhanced catalytic activity and selectivity is challenging, with conflicting arguments often presented based on indirect evidence. Here, we separate the metal from the support by a controlled distance while maintaining the ability to promote defects via the use of carbon nanotube hydrogen highways. As illustrative cases, we use this approach to show that the selective transformation of furfural to methylfuran over Pd/TiO2 occurs at the Pd-TiO2 interface while anisole conversion to phenol and cresol over Cu/TiO2 is facilitated by exposed Ti3+ cations on the support. This approach can be used to clarify many conflicting arguments in the literature.

Authors:
; ; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE; National Science Foundation (NSF)
OSTI Identifier:
1470788
Alternate Identifier(s):
OSTI ID: 1601877
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 9 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Briggs, Nicholas M., Barrett, Lawrence, Wegener, Evan C., Herrera, Leidy V., Gomez, Laura A., Miller, Jeffrey T., and Crossley, Steven P. Identification of active sites on supported metal catalysts with carbon nanotube hydrogen highways. United Kingdom: N. p., 2018. Web. doi:10.1038/s41467-018-06100-9.
Briggs, Nicholas M., Barrett, Lawrence, Wegener, Evan C., Herrera, Leidy V., Gomez, Laura A., Miller, Jeffrey T., & Crossley, Steven P. Identification of active sites on supported metal catalysts with carbon nanotube hydrogen highways. United Kingdom. doi:10.1038/s41467-018-06100-9.
Briggs, Nicholas M., Barrett, Lawrence, Wegener, Evan C., Herrera, Leidy V., Gomez, Laura A., Miller, Jeffrey T., and Crossley, Steven P. Thu . "Identification of active sites on supported metal catalysts with carbon nanotube hydrogen highways". United Kingdom. doi:10.1038/s41467-018-06100-9.
@article{osti_1470788,
title = {Identification of active sites on supported metal catalysts with carbon nanotube hydrogen highways},
author = {Briggs, Nicholas M. and Barrett, Lawrence and Wegener, Evan C. and Herrera, Leidy V. and Gomez, Laura A. and Miller, Jeffrey T. and Crossley, Steven P.},
abstractNote = {Catalysts consisting of metal particles supported on reducible oxides exhibit promising activity and selectivity for a variety of current and emerging industrial processes. Enhanced catalytic activity can arise from direct contact between the support and the metal or from metal-induced promoter effects on the oxide. Discovering the source of enhanced catalytic activity and selectivity is challenging, with conflicting arguments often presented based on indirect evidence. Here, we separate the metal from the support by a controlled distance while maintaining the ability to promote defects via the use of carbon nanotube hydrogen highways. As illustrative cases, we use this approach to show that the selective transformation of furfural to methylfuran over Pd/TiO2 occurs at the Pd-TiO2 interface while anisole conversion to phenol and cresol over Cu/TiO2 is facilitated by exposed Ti3+ cations on the support. This approach can be used to clarify many conflicting arguments in the literature.},
doi = {10.1038/s41467-018-06100-9},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United Kingdom},
year = {2018},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1038/s41467-018-06100-9

Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Freestanding foils of nanotube arrays fused with metals
journal, July 2014

  • Poenitzsch, Vasiliki Z.; Slinker, Keith A.; Miles, Dustin W.
  • Journal of Materials Science, Vol. 49, Issue 20
  • DOI: 10.1007/s10853-014-8414-x

A model of metal-oxide support interaction for Rh on TiO2
journal, August 1983


Kinetics and Mechanism of Ketonization of Acetic Acid on Ru/TiO2 Catalyst
journal, November 2013


Improvement of Oxidation Resistance of Ultrafine Copper Powders by Phosphating Treatment
journal, April 1997

  • Zhao, Bin; Liu, Zhijie; Zhang, Zongtao
  • Journal of Solid State Chemistry, Vol. 130, Issue 1
  • DOI: 10.1006/jssc.1997.7276

Directing Reaction Pathways through Controlled Reactant Binding at Pd-TiO 2 Interfaces
journal, May 2017

  • Zhang, Jing; Wang, Bingwen; Nikolla, Eranda
  • Angewandte Chemie International Edition, Vol. 56, Issue 23
  • DOI: 10.1002/anie.201703669

Optical Properties and Oxidation of Evaporated Titanium Films*
journal, January 1957

  • Hass, Georg; Bradford, Alan P.
  • Journal of the Optical Society of America, Vol. 47, Issue 2
  • DOI: 10.1364/JOSA.47.000125

Conversion of furfural and 2-methylpentanal on Pd/SiO2 and Pd–Cu/SiO2 catalysts
journal, May 2011


Wafer-Scale Transfer of Vertically Aligned Carbon Nanotube Arrays
journal, December 2014

  • Wang, Miao; Li, Taotao; Yao, Yagang
  • Journal of the American Chemical Society, Vol. 136, Issue 52
  • DOI: 10.1021/ja511373g

Experimental and First-Principles Evidence for Interfacial Activity of Ru/TiO 2 for the Direct Conversion of m -Cresol to Toluene
journal, July 2017

  • Omotoso, Taiwo O.; Baek, Byeongjin; Grabow, Lars C.
  • ChemCatChem, Vol. 9, Issue 14
  • DOI: 10.1002/cctc.201700157

Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide
journal, January 1978

  • Tauster, S. J.; Fung, S. C.; Garten, R. L.
  • Journal of the American Chemical Society, Vol. 100, Issue 1
  • DOI: 10.1021/ja00469a029

Mechanistic Study on Hydrogen Spillover onto Graphitic Carbon Materials
journal, December 2007

  • Chen, Liang; Cooper, Alan C.; Pez, Guido P.
  • The Journal of Physical Chemistry C, Vol. 111, Issue 51
  • DOI: 10.1021/jp074920g

Oxidation of titanium between 25°C and 400°C
journal, July 1973


Cycloaddition of Biomass-Derived Furans for Catalytic Production of Renewable p -Xylene
journal, April 2012

  • Williams, C. Luke; Chang, Chun-Chih; Do, Phuong
  • ACS Catalysis, Vol. 2, Issue 6
  • DOI: 10.1021/cs300011a

Selective conversion of furfural to methylfuran over silica-supported NiFe bimetallic catalysts
journal, November 2011


Hydrogen Spillover in Pt-Single-Walled Carbon Nanotube Composites: Formation of Stable C−H Bonds
journal, April 2011

  • Bhowmick, Ranadeep; Rajasekaran, Srivats; Friebel, Daniel
  • Journal of the American Chemical Society, Vol. 133, Issue 14
  • DOI: 10.1021/ja200403m

Effects of Dispersion and Metal-Metal Oxide Interactions on Fischer-Tropsch Synthesis over Ru/TiO2 and TiO2-Promoted Ru/SiO2
journal, December 1994


Effect of Surface Oxygen Groups in Carbons on Hydrogen Storage by Spillover
journal, March 2009

  • Wang, Lifeng; Yang, Frances H.; Yang, Ralph T.
  • Industrial & Engineering Chemistry Research, Vol. 48, Issue 6
  • DOI: 10.1021/ie8014507

A mechanistic study of hydrogen spillover in MoO 3 and carbon-based graphitic materials
journal, January 2008


Ketonization of Carboxylic Acids: Mechanisms, Catalysts, and Implications for Biomass Conversion
journal, October 2013

  • Pham, Tu N.; Sooknoi, Tawan; Crossley, Steven P.
  • ACS Catalysis, Vol. 3, Issue 11
  • DOI: 10.1021/cs400501h

DFT Study of Hydrogen Storage by Spillover on Graphite with Oxygen Surface Groups
journal, October 2009

  • Psofogiannakis, George M.; Froudakis, George E.
  • Journal of the American Chemical Society, Vol. 131, Issue 42
  • DOI: 10.1021/ja906159p

A Sinter-Resistant Catalytic System Based on Platinum Nanoparticles Supported on TiO2 Nanofibers and Covered by Porous Silica
journal, September 2010

  • Dai, Yunqian; Lim, Byungkwon; Yang, Yong
  • Angewandte Chemie International Edition, Vol. 49, Issue 44
  • DOI: 10.1002/anie.201001839

Effective hydrodeoxygenation of biomass-derived oxygenates into unsaturated hydrocarbons by MoO3 using low H2 pressures
journal, January 2013

  • Prasomsri, Teerawit; Nimmanwudipong, Tarit; Román-Leshkov, Yuriy
  • Energy & Environmental Science, Vol. 6, Issue 6, p. 1732-1738
  • DOI: 10.1039/c3ee24360e

Selective Amplification of CO Bond Hydrogenation on Pt/TiO 2 : Catalytic Reaction and Sum-Frequency Generation Vibrational Spectroscopy Studies of Crotonaldehyde Hydrogenation
journal, February 2014

  • Kennedy, Griffin; Baker, L. Robert; Somorjai, Gabor A.
  • Angewandte Chemie International Edition, Vol. 53, Issue 13
  • DOI: 10.1002/anie.201400081

Isothermal Reduction Kinetics of Titanium Dioxide-Based Materials
journal, February 1997

  • Rekoske, James E.; Barteau, Mark A.
  • The Journal of Physical Chemistry B, Vol. 101, Issue 7
  • DOI: 10.1021/jp9620025

Strong Metal–Support Interactions Enhance the Pairwise Selectivity of Parahydrogen Addition over Ir/TiO 2
journal, January 2016


The Effect of Size-Dependent Nanoparticle Energetics on Catalyst Sintering
journal, October 2002


Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts
journal, July 2013


WinXAS a Program for X-ray Absorption Spectroscopy Data Analysis under MS-Windows
journal, March 1998


Oxidation and protection in copper and copper alloy thin films
journal, September 1991

  • Li, Jian; Mayer, J. W.; Colgan, E. G.
  • Journal of Applied Physics, Vol. 70, Issue 5
  • DOI: 10.1063/1.349344

A Sinter-Resistant Catalytic System Based on Platinum Nanoparticles Supported on TiO2 Nanofibers and Covered by Porous Silica
journal, September 2010


    Works referencing / citing this record:

    Cooperative Co 0 /Co II Sites Stabilized by a Perovskite Matrix Enable Selective C−O and C−C bond Hydrogenolysis of Oxygenated Arenes
    journal, April 2019

    • Shetty, Manish; Zanchet, Daniela; Green, William H.
    • ChemSusChem, Vol. 12, Issue 10
    • DOI: 10.1002/cssc.201900664

    Origin of synergistic effects in bicomponent cobalt oxide-platinum catalysts for selective hydrogenation reaction
    journal, September 2019


    Cobalt-Based Fischer–Tropsch Synthesis: A Kinetic Evaluation of Metal–Support Interactions Using an Inverse Model System
    journal, September 2019

    • Petersen, Anna P.; Claeys, Michael; Kooyman, Patricia J.
    • Catalysts, Vol. 9, Issue 10
    • DOI: 10.3390/catal9100794