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Title: Gold-Copper Nanoparticles: Nanostructural Evolution and Bifunctional Catalytic Sites

Abstract

Understanding of the atomic-scale structure is essential for exploiting the unique catalytic properties of any nanoalloy catalyst. This report describes novel findings of an investigation of the nanoscale alloying of gold-copper (AuCu) nanoparticles and its impact on the surface catalytic functions. Two pathways have been explored for the formation of AuCu nanoparticles of different compositons, including wet chemical synthesis from mixed Au- and Cu-precursor molecules, and nanoscale alloying via an evolution of mixed Au- and Cu-precursor nanoparticles near the nanoscale melting temperatures. For the evolution of mixed precursor nanoparticles, synchrotron x-ray based in-situ real time XRD was used to monitor the structural changes, revealing nanoscale alloying and reshaping towards an fcc-type nanoalloy (particle or cube) via a partial melting–resolidification mechanism. The nanoalloys supported on carbon or silica were characterized by in-situ high-energy XRD/PDFs, revealing an intriguing lattice "expanding-shrinking" phenomenon depending on whether the catalyst is thermochemically processed under oxidative or reductive atmosphere. This type of controllable structural changes is found to play an important role in determining the catalytic activity of the catalysts for carbon monoxide oxidation reaction. The tunable catalytic activities of the nanoalloys under thermochemically oxidative and reductive atmospheres are also discussed in terms of the bifunctional sitesmore » and the surface oxygenated metal species for carbon monoxide and oxygen activation.« less

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1060133
Report Number(s):
PNNL-SA-89261
46204; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Chemistry of Materials, 24(24):4662-4674
Additional Journal Information:
Journal Name: Chemistry of Materials, 24(24):4662-4674
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Yin, Jun, Shan, Shiyao, Yang, Lefu, Mott, Derrick, Malis, Oana, Petkov, Valeri, Cai, Fan, Ng, Mei, Luo, Jin, Chen, Bing H, Engelhard, Mark H, and Zhong, Chuan-Jian. Gold-Copper Nanoparticles: Nanostructural Evolution and Bifunctional Catalytic Sites. United States: N. p., 2012. Web. doi:10.1021/cm302097c.
Yin, Jun, Shan, Shiyao, Yang, Lefu, Mott, Derrick, Malis, Oana, Petkov, Valeri, Cai, Fan, Ng, Mei, Luo, Jin, Chen, Bing H, Engelhard, Mark H, & Zhong, Chuan-Jian. Gold-Copper Nanoparticles: Nanostructural Evolution and Bifunctional Catalytic Sites. United States. https://doi.org/10.1021/cm302097c
Yin, Jun, Shan, Shiyao, Yang, Lefu, Mott, Derrick, Malis, Oana, Petkov, Valeri, Cai, Fan, Ng, Mei, Luo, Jin, Chen, Bing H, Engelhard, Mark H, and Zhong, Chuan-Jian. Wed . "Gold-Copper Nanoparticles: Nanostructural Evolution and Bifunctional Catalytic Sites". United States. https://doi.org/10.1021/cm302097c.
@article{osti_1060133,
title = {Gold-Copper Nanoparticles: Nanostructural Evolution and Bifunctional Catalytic Sites},
author = {Yin, Jun and Shan, Shiyao and Yang, Lefu and Mott, Derrick and Malis, Oana and Petkov, Valeri and Cai, Fan and Ng, Mei and Luo, Jin and Chen, Bing H and Engelhard, Mark H and Zhong, Chuan-Jian},
abstractNote = {Understanding of the atomic-scale structure is essential for exploiting the unique catalytic properties of any nanoalloy catalyst. This report describes novel findings of an investigation of the nanoscale alloying of gold-copper (AuCu) nanoparticles and its impact on the surface catalytic functions. Two pathways have been explored for the formation of AuCu nanoparticles of different compositons, including wet chemical synthesis from mixed Au- and Cu-precursor molecules, and nanoscale alloying via an evolution of mixed Au- and Cu-precursor nanoparticles near the nanoscale melting temperatures. For the evolution of mixed precursor nanoparticles, synchrotron x-ray based in-situ real time XRD was used to monitor the structural changes, revealing nanoscale alloying and reshaping towards an fcc-type nanoalloy (particle or cube) via a partial melting–resolidification mechanism. The nanoalloys supported on carbon or silica were characterized by in-situ high-energy XRD/PDFs, revealing an intriguing lattice "expanding-shrinking" phenomenon depending on whether the catalyst is thermochemically processed under oxidative or reductive atmosphere. This type of controllable structural changes is found to play an important role in determining the catalytic activity of the catalysts for carbon monoxide oxidation reaction. The tunable catalytic activities of the nanoalloys under thermochemically oxidative and reductive atmospheres are also discussed in terms of the bifunctional sites and the surface oxygenated metal species for carbon monoxide and oxygen activation.},
doi = {10.1021/cm302097c},
url = {https://www.osti.gov/biblio/1060133}, journal = {Chemistry of Materials, 24(24):4662-4674},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {12}
}