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

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. Furthermore, the results highlight the power of super-resolution catalysis imaging in gaining insights that could help improve nanocatalysts.

Authors:
 [1];  [1]; ORCiD logo [1];  [2];  [2]; ORCiD logo [1]
  1. Cornell Univ., Ithaca, NY (United States)
  2. Cornell Univ., Ithaca, NY (United States); Colorado State Univ., Fort Collins, CO (United States)
Publication Date:
Research Org.:
Cornell Univ., Ithaca, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1406929
Alternate Identifier(s):
OSTI ID: 1417631
Grant/Contract Number:
SC0004911; SC0001057
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 3; Journal Issue: 11; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
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. doi: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. doi: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. Furthermore, 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 at 10.1021/acscentsci.7b00377

Save / Share: