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Title: Gold nanoparticle-catalyzed reduction in a model system: Quantitative determination of reactive heterogeneity of a supported nanoparticle surface

Abstract

Kinetic poisoning experiments employing organic ligands were conducted using a gold nanoparticle–catalyzed reaction consisting of the reduction of resazurin to resorufin. The kinetic contributions of three distinct types of sites along with the number density of each of these site types during reaction were determined. The calculated number densities of each of the three types of sites, hypothesized to be corners, edges, and terraces, correlates well with atomic-resolution micrographs of the supported gold nanoparticles, obtained using aberration-corrected transmission electron microscopy and with predictions based on geometric models of idealized gold nanoparticles. The most active sites comprising 1% of the surface atoms exhibit at least 30% of the total activity of the catalyst for resazurin reduction. The selective mechanical blocking of surface sites on nanoparticles, particularly undercoordinated sites, paves the way for novel approaches utilizing organic ligands to quantify the activity of different active sites and control catalysis on metal surfaces. This work was supported in part by the Laboratory Directed Research and Development program at the Pacific Northwest National Laboratory (PNNL). The aberration-corrected electron microscopy was performed in the William R. Wiley Environmental Molecular Sciences Laboratory, a U.S. Department of Energy (DOE) national scientific user facility located at PNNL andmore » funded by BER. PNNL is operated by Battelle for the U.S. DOE under contract DE-AC05-76RL01830.« less

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1059196
Report Number(s):
PNNL-SA-91255
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis, 295:115-121
Additional Journal Information:
Journal Name: Journal of Catalysis, 295:115-121
Country of Publication:
United States
Language:
English
Subject:
gold nanoparticle; catalysis; corner; edge; coordinative unsaturation; resazurin; electron transfer

Citation Formats

Nigra, Michael M., Arslan, Ilke, and Katz, Alexander. Gold nanoparticle-catalyzed reduction in a model system: Quantitative determination of reactive heterogeneity of a supported nanoparticle surface. United States: N. p., 2012. Web. doi:10.1016/j.jcat.2012.08.001.
Nigra, Michael M., Arslan, Ilke, & Katz, Alexander. Gold nanoparticle-catalyzed reduction in a model system: Quantitative determination of reactive heterogeneity of a supported nanoparticle surface. United States. doi:10.1016/j.jcat.2012.08.001.
Nigra, Michael M., Arslan, Ilke, and Katz, Alexander. Thu . "Gold nanoparticle-catalyzed reduction in a model system: Quantitative determination of reactive heterogeneity of a supported nanoparticle surface". United States. doi:10.1016/j.jcat.2012.08.001.
@article{osti_1059196,
title = {Gold nanoparticle-catalyzed reduction in a model system: Quantitative determination of reactive heterogeneity of a supported nanoparticle surface},
author = {Nigra, Michael M. and Arslan, Ilke and Katz, Alexander},
abstractNote = {Kinetic poisoning experiments employing organic ligands were conducted using a gold nanoparticle–catalyzed reaction consisting of the reduction of resazurin to resorufin. The kinetic contributions of three distinct types of sites along with the number density of each of these site types during reaction were determined. The calculated number densities of each of the three types of sites, hypothesized to be corners, edges, and terraces, correlates well with atomic-resolution micrographs of the supported gold nanoparticles, obtained using aberration-corrected transmission electron microscopy and with predictions based on geometric models of idealized gold nanoparticles. The most active sites comprising 1% of the surface atoms exhibit at least 30% of the total activity of the catalyst for resazurin reduction. The selective mechanical blocking of surface sites on nanoparticles, particularly undercoordinated sites, paves the way for novel approaches utilizing organic ligands to quantify the activity of different active sites and control catalysis on metal surfaces. This work was supported in part by the Laboratory Directed Research and Development program at the Pacific Northwest National Laboratory (PNNL). The aberration-corrected electron microscopy was performed in the William R. Wiley Environmental Molecular Sciences Laboratory, a U.S. Department of Energy (DOE) national scientific user facility located at PNNL and funded by BER. PNNL is operated by Battelle for the U.S. DOE under contract DE-AC05-76RL01830.},
doi = {10.1016/j.jcat.2012.08.001},
journal = {Journal of Catalysis, 295:115-121},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {11}
}