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Title: Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging

Abstract

Compared with their monometallic counterparts, bimetallic nanoparticles often show enhanced catalytic activity associated with the bimetallic interface. Direct quantitation of catalytic activity at the bimetallic interface is important for understanding the enhancement mechanism, but challenging experimentally. Here using single-molecule super-resolution catalysis imaging in correlation with electron microscopy, we report the first quantitative visualization of enhanced bimetallic activity within single bimetallic nanoparticles. We focus on heteronuclear bimetallic PdAu nanoparticles that present a well-defined Pd–Au bimetallic interface in catalyzing a photodriven fluorogenic disproportionation reaction. Our approach also enables a direct comparison between the bimetallic and monometallic regions within the same nanoparticle. Theoretical calculations further provide insights into the electronic nature of N–O bond activation of the reactant (resazurin) adsorbed on bimetallic sites. Subparticle activity correlation between bimetallic enhancement and monometallic activity suggests that the favorable locations to construct bimetallic sites are those monometallic sites with higher activity, leading to a strategy for making effective bimetallic nanocatalysts. The results highlight the power of super-resolution catalysis imaging in gaining insights that could help improve nanocatalysts.

Authors:
 [1];  [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]
  1. Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, United States
Publication Date:
Research Org.:
Cornell Univ., Ithaca, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research in Extreme Environments (EFree)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1406929
Alternate Identifier(s):
OSTI ID: 1417631; OSTI ID: 1507709
Grant/Contract Number:  
SC0001057; SC0004911
Resource Type:
Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Name: ACS Central Science Journal Volume: 3 Journal Issue: 11; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Guanqun, Zou, Ningmu, Chen, Bo, Sambur, Justin B., Choudhary, Eric, and Chen, Peng. Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging. United States: N. p., 2017. Web. doi:10.1021/acscentsci.7b00377.
Chen, Guanqun, Zou, Ningmu, Chen, Bo, Sambur, Justin B., Choudhary, Eric, & Chen, Peng. Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging. United States. https://doi.org/10.1021/acscentsci.7b00377
Chen, Guanqun, Zou, Ningmu, Chen, Bo, Sambur, Justin B., Choudhary, Eric, and Chen, Peng. Wed . "Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging". United States. https://doi.org/10.1021/acscentsci.7b00377.
@article{osti_1406929,
title = {Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging},
author = {Chen, Guanqun and Zou, Ningmu and Chen, Bo and Sambur, Justin B. and Choudhary, Eric and Chen, Peng},
abstractNote = {Compared with their monometallic counterparts, bimetallic nanoparticles often show enhanced catalytic activity associated with the bimetallic interface. Direct quantitation of catalytic activity at the bimetallic interface is important for understanding the enhancement mechanism, but challenging experimentally. Here using single-molecule super-resolution catalysis imaging in correlation with electron microscopy, we report the first quantitative visualization of enhanced bimetallic activity within single bimetallic nanoparticles. We focus on heteronuclear bimetallic PdAu nanoparticles that present a well-defined Pd–Au bimetallic interface in catalyzing a photodriven fluorogenic disproportionation reaction. Our approach also enables a direct comparison between the bimetallic and monometallic regions within the same nanoparticle. Theoretical calculations further provide insights into the electronic nature of N–O bond activation of the reactant (resazurin) adsorbed on bimetallic sites. Subparticle activity correlation between bimetallic enhancement and monometallic activity suggests that the favorable locations to construct bimetallic sites are those monometallic sites with higher activity, leading to a strategy for making effective bimetallic nanocatalysts. The results highlight the power of super-resolution catalysis imaging in gaining insights that could help improve nanocatalysts.},
doi = {10.1021/acscentsci.7b00377},
journal = {ACS Central Science},
number = 11,
volume = 3,
place = {United States},
year = {Wed Nov 01 00:00:00 EDT 2017},
month = {Wed Nov 01 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acscentsci.7b00377

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