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

Title: Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: Structure-activity relationship

Abstract

Uniform Au nanoparticles (~2 nm) with narrow size-distribution (standard deviation: 0.5–0.6 nm) supported on both hydroxylated (Fe_OH) and dehydrated iron oxide (Fe_O) have been prepared by either deposition-precipitation (DP) or colloidal-deposition (CD) methods. Different structural and textural characterizations were applied to the dried, calcined and used gold-iron oxide samples. The transmission electron microscopy (TEM) and high-resolution TEM (HRTEM) described the high homogeneity in the supported Au nanoparticles. The ex-situ and in-situ X-ray absorption fine structure (XAFS) characterization monitored the electronic and short-range local structure of active gold species. The synchrotron-based in-situ X-ray diffraction (XRD), together with the corresponding temperature-programmed reduction by hydrogen (H₂-TPR), indicated a structural evolution of the iron-oxide supports, correlating to their reducibility. An inverse order of catalytic activity between DP (Au/Fe_OH < Au/Fe_O) and CD (Au/Fe_OH > Au/Fe_O) was observed. Effective gold-support interaction results in a high activity for gold nanoparticles, locally generated by the sintering of dispersed Au atoms on the oxide support in the DP synthesis, while a hydroxylated surface favors the reactivity of externally introduced Au nanoparticles on Fe_OH support for the CD approach. This work reveals why differences in the synthetic protocol translate to differences in the catalytic performance of Au/FeOx catalysts withmore » very similar structural characteristics in CO oxidation.« less

Authors:
 [1];  [2];  [3];  [1];  [4];  [4];  [2];  [4];  [2];  [1];  [1];  [3]
  1. Shandong Univ., Jinan (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Max-Planck Institut fur Kohlenforschung (Germany)
  4. Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1213360
Report Number(s):
BNL-108165-2015-JA
Journal ID: ISSN 2040-3364; NANOHL; R&D Project: CO009; KC0302010
Grant/Contract Number:  
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 7; Journal Issue: 11; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; gold catalyst; iron oxide; CO oxidation; in-situ x-ray technique; metal-support interaction

Citation Formats

Guo, Yu, Senanayake, Sanjaya, Gu, Dong, Jin, Zhao, Du, Pei -Pei, Si, Rui, Xu, Wen -Qian, Huang, Yu -Ying, Tao, Jing, Song, Qi -Sheng, Jia, Chun -Jia, and Schueth, Ferdi. Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: Structure-activity relationship. United States: N. p., 2015. Web. doi:10.1039/c4nr06967f.
Guo, Yu, Senanayake, Sanjaya, Gu, Dong, Jin, Zhao, Du, Pei -Pei, Si, Rui, Xu, Wen -Qian, Huang, Yu -Ying, Tao, Jing, Song, Qi -Sheng, Jia, Chun -Jia, & Schueth, Ferdi. Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: Structure-activity relationship. United States. https://doi.org/10.1039/c4nr06967f
Guo, Yu, Senanayake, Sanjaya, Gu, Dong, Jin, Zhao, Du, Pei -Pei, Si, Rui, Xu, Wen -Qian, Huang, Yu -Ying, Tao, Jing, Song, Qi -Sheng, Jia, Chun -Jia, and Schueth, Ferdi. 2015. "Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: Structure-activity relationship". United States. https://doi.org/10.1039/c4nr06967f. https://www.osti.gov/servlets/purl/1213360.
@article{osti_1213360,
title = {Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: Structure-activity relationship},
author = {Guo, Yu and Senanayake, Sanjaya and Gu, Dong and Jin, Zhao and Du, Pei -Pei and Si, Rui and Xu, Wen -Qian and Huang, Yu -Ying and Tao, Jing and Song, Qi -Sheng and Jia, Chun -Jia and Schueth, Ferdi},
abstractNote = {Uniform Au nanoparticles (~2 nm) with narrow size-distribution (standard deviation: 0.5–0.6 nm) supported on both hydroxylated (Fe_OH) and dehydrated iron oxide (Fe_O) have been prepared by either deposition-precipitation (DP) or colloidal-deposition (CD) methods. Different structural and textural characterizations were applied to the dried, calcined and used gold-iron oxide samples. The transmission electron microscopy (TEM) and high-resolution TEM (HRTEM) described the high homogeneity in the supported Au nanoparticles. The ex-situ and in-situ X-ray absorption fine structure (XAFS) characterization monitored the electronic and short-range local structure of active gold species. The synchrotron-based in-situ X-ray diffraction (XRD), together with the corresponding temperature-programmed reduction by hydrogen (H₂-TPR), indicated a structural evolution of the iron-oxide supports, correlating to their reducibility. An inverse order of catalytic activity between DP (Au/Fe_OH < Au/Fe_O) and CD (Au/Fe_OH > Au/Fe_O) was observed. Effective gold-support interaction results in a high activity for gold nanoparticles, locally generated by the sintering of dispersed Au atoms on the oxide support in the DP synthesis, while a hydroxylated surface favors the reactivity of externally introduced Au nanoparticles on Fe_OH support for the CD approach. This work reveals why differences in the synthetic protocol translate to differences in the catalytic performance of Au/FeOx catalysts with very similar structural characteristics in CO oxidation.},
doi = {10.1039/c4nr06967f},
url = {https://www.osti.gov/biblio/1213360}, journal = {Nanoscale},
issn = {2040-3364},
number = 11,
volume = 7,
place = {United States},
year = {Mon Jan 12 00:00:00 EST 2015},
month = {Mon Jan 12 00:00:00 EST 2015}
}

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

Citation Metrics:
Cited by: 43 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Moisture Effect on CO Oxidation over Au/TiO2 Catalyst
journal, July 2001


Strong Metal–Support Interactions between Gold Nanoparticles and ZnO Nanorods in CO Oxidation
journal, June 2012


Stabilized Gold Nanoparticles on Ceria Nanorods by Strong Interfacial Anchoring
journal, December 2012


Gold Catalysis
journal, December 2006


The Role of Pore Size and Structure on the Thermal Stability of Gold Nanoparticles within Mesoporous Silica
journal, February 2005


Catalysis by Supported Gold:  Correlation between Catalytic Activity for CO Oxidation and Oxidation States of Gold
journal, March 2004


Gold Nanoparticles Supported on Carbon Nitride: Influence of Surface Hydroxyls on Low Temperature Carbon Monoxide Oxidation
journal, April 2012


Role of gold cations in the oxidation of carbon monoxide catalyzed by iron oxide-supported gold
journal, August 2006


Characterization and reactivity in CO oxidation of gold nanoparticles supported on TiO2 prepared by deposition-precipitation with NaOH and urea
journal, March 2004


Reaction-Relevant Gold Structures in the Low Temperature Water-Gas Shift Reaction on Au-CeO 2
journal, August 2008


Low-Temperature Oxidation of CO over Gold Supported on TiO2, α-Fe2O3, and Co3O4
journal, November 1993


Highly Active Iron Oxide Supported Gold Catalysts for CO Oxidation: How Small Must the Gold Nanoparticles Be?
journal, July 2010


Very Low Temperature CO Oxidation over Colloidally Deposited Gold Nanoparticles on Mg(OH) 2 and MgO
journal, February 2010


Support Effect in High Activity Gold Catalysts for CO Oxidation
journal, January 2006


Evolution of gold structure during thermal treatment of Au/FeOx catalysts revealed by aberration-corrected electron microscopy
journal, April 2009


Nanocrystalline CeO2 Increases the Activity of Au for CO Oxidation by Two Orders of Magnitude
journal, May 2004


Time Resolved in Situ XAFS Study of the Electrochemical Oxygen Intercalation in SrFeO 2.5 Brownmillerite Structure: Comparison with the Homologous SrCoO 2.5 System
journal, September 2010


Gold-catalysed oxidation of carbon monoxide
journal, June 2000


Increasing the Number of Oxygen Vacancies on TiO2 by Doping with Iron Increases the Activity of Supported Gold for CO Oxidation
journal, September 2007


CO Oxidation over Supported Gold Catalysts—“Inert” and “Active” Support Materials and Their Role for the Oxygen Supply during Reaction
journal, January 2001


Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation
journal, September 2008


Reactive oxygen on a Au/TiO2 supported catalyst
journal, May 2009


Structure and oxidation state of gold on different supports under various CO oxidation conditions
journal, June 2006


Comparison of the activity of Au/CeO2 and Au/Fe2O3 catalysts for the CO oxidation and the water-gas shift reactions
journal, June 2007


Influence of Support Hydroxides on the Catalytic Activity of Oxidized Gold Clusters
journal, March 2010


Works referencing / citing this record:

Monolithic Au/CeO 2 nanorod framework catalyst prepared by dealloying for low-temperature CO oxidation
journal, January 2018


Geometrical Structure of the Gold-Iron(III) Oxide Interfacial Perimeter for CO Oxidation
journal, July 2018


Size‐Dependency of Gold Nanoparticles on TiO 2 for CO Oxidation
journal, September 2018


Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation
journal, September 2016


Perspective of Surfactant‐Free Colloidal Nanoparticles in Heterogeneous Catalysis
journal, August 2019


Geometrical Structure of the Gold-Iron(III) Oxide Interfacial Perimeter for CO Oxidation
journal, July 2018