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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/FeO x catalystsmore » with 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) (SC-22)
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:
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. 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, and Schueth, Ferdi. Mon . "Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: Structure-activity relationship". United States. doi: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},
journal = {Nanoscale},
number = 11,
volume = 7,
place = {United States},
year = {2015},
month = {1}
}

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