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

Title: In Situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles

Abstract

Multielectron transfer processes are crucially important in energy and biological science but require favorable catalysts to achieve fast kinetics. Nanostructuring catalysts can dramatically improve their properties, which can be difficult to understand due to strain- and size-dependent thermodynamics, the influence of defects, and substrate-dependent activities. Here, we report three-dimensional (3D) imaging of single gold nanoparticles during catalysis of ascorbic acid decomposition using Bragg coherent diffractive imaging (BCDI). Local strains were measured in single nanoparticles and modeled using reactive molecular dynamics (RMD) simulations and finite element analysis (FEA) simulations. RMD reveals the pathway for local strain generation in the gold lattice: chemisorption of hydroxyl ions. FEA reveals that the RMD results are transferable to the nanocrystal sizes studied in the experiment. Our study probes the strain-activity connection and opens a powerful avenue for theoretical and experimental studies of nanocrystal catalysis.

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1330099
DOE Contract Number:
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Physical Chemistry Letters; Journal Volume: 7; Journal Issue: 15
Country of Publication:
United States
Language:
English

Citation Formats

Ulvestad, Andrew, Sasikumar, Kiran, Kim, Jong Woo, Harder, Ross, Maxey, Evan, Clark, Jesse N., Narayanan, Badri, Deshmukh, Sanket A., Ferrier, Nicola, Mulvaney, Paul, Sankaranarayanan, Subramanian K. R. S., and Shpyrko, Oleg G. In Situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles. United States: N. p., 2016. Web. doi:10.1021/acs.jpclett.6b01038.
Ulvestad, Andrew, Sasikumar, Kiran, Kim, Jong Woo, Harder, Ross, Maxey, Evan, Clark, Jesse N., Narayanan, Badri, Deshmukh, Sanket A., Ferrier, Nicola, Mulvaney, Paul, Sankaranarayanan, Subramanian K. R. S., & Shpyrko, Oleg G. In Situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles. United States. doi:10.1021/acs.jpclett.6b01038.
Ulvestad, Andrew, Sasikumar, Kiran, Kim, Jong Woo, Harder, Ross, Maxey, Evan, Clark, Jesse N., Narayanan, Badri, Deshmukh, Sanket A., Ferrier, Nicola, Mulvaney, Paul, Sankaranarayanan, Subramanian K. R. S., and Shpyrko, Oleg G. Thu . "In Situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles". United States. doi:10.1021/acs.jpclett.6b01038.
@article{osti_1330099,
title = {In Situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles},
author = {Ulvestad, Andrew and Sasikumar, Kiran and Kim, Jong Woo and Harder, Ross and Maxey, Evan and Clark, Jesse N. and Narayanan, Badri and Deshmukh, Sanket A. and Ferrier, Nicola and Mulvaney, Paul and Sankaranarayanan, Subramanian K. R. S. and Shpyrko, Oleg G.},
abstractNote = {Multielectron transfer processes are crucially important in energy and biological science but require favorable catalysts to achieve fast kinetics. Nanostructuring catalysts can dramatically improve their properties, which can be difficult to understand due to strain- and size-dependent thermodynamics, the influence of defects, and substrate-dependent activities. Here, we report three-dimensional (3D) imaging of single gold nanoparticles during catalysis of ascorbic acid decomposition using Bragg coherent diffractive imaging (BCDI). Local strains were measured in single nanoparticles and modeled using reactive molecular dynamics (RMD) simulations and finite element analysis (FEA) simulations. RMD reveals the pathway for local strain generation in the gold lattice: chemisorption of hydroxyl ions. FEA reveals that the RMD results are transferable to the nanocrystal sizes studied in the experiment. Our study probes the strain-activity connection and opens a powerful avenue for theoretical and experimental studies of nanocrystal catalysis.},
doi = {10.1021/acs.jpclett.6b01038},
journal = {Journal of Physical Chemistry Letters},
number = 15,
volume = 7,
place = {United States},
year = {Thu Aug 04 00:00:00 EDT 2016},
month = {Thu Aug 04 00:00:00 EDT 2016}
}