Surface faceting and elemental diffusion behaviour at atomic scale for alloy nanoparticles during in situ annealing
Abstract
The catalytic performance of nanoparticles is primarily determined by the precise nature of the surface and near-surface atomic configurations, which can be tailored by post-synthesis annealing effectively and straightforwardly. Understanding the complete dynamic response of surface structure and chemistry to thermal treatments at the atomic scale is imperative for the rational design of catalyst nanoparticles. Here, by tracking the same individual Pt3Co nanoparticles during in situ annealing in a scanning transmission electron microscope, we directly discern five distinct stages of surface elemental rearrangements in Pt3Co nanoparticles at the atomic scale: initial random (alloy) elemental distribution; surface platinum-skin-layer formation; nucleation of structurally ordered domains; ordered framework development and, finally, initiation of amorphization. Furthermore, a comprehensive interplay among phase evolution, surface faceting and elemental inter-diffusion is revealed, and supported by atomistic simulations. In conlcusion, this work may pave the way towards designing catalysts through post-synthesis annealing for optimized catalytic performance.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- John Hopkins Univ., Baltimore, MD (United States)
- Univ. of Pittsburgh, Pittsburgh, PA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1249113
- Alternate Identifier(s):
- OSTI ID: 1271885
- Grant/Contract Number:
- AC02-06CH11357; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 8925; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; chemical sciences; catalysis; materials science; 36 MATERIALS SCIENCE
Citation Formats
Chi, Miaofang, Wang, Chao, Lei, Yinkai, Wang, Guofeng, Li, Dongguo, More, Karren L., Lupini, Andrew, Allard, Lawrence F., Markovic, Nenad M., and Stamenkovic, Vojislav R. Surface faceting and elemental diffusion behaviour at atomic scale for alloy nanoparticles during in situ annealing. United States: N. p., 2015.
Web. doi:10.1038/ncomms9925.
Chi, Miaofang, Wang, Chao, Lei, Yinkai, Wang, Guofeng, Li, Dongguo, More, Karren L., Lupini, Andrew, Allard, Lawrence F., Markovic, Nenad M., & Stamenkovic, Vojislav R. Surface faceting and elemental diffusion behaviour at atomic scale for alloy nanoparticles during in situ annealing. United States. https://doi.org/10.1038/ncomms9925
Chi, Miaofang, Wang, Chao, Lei, Yinkai, Wang, Guofeng, Li, Dongguo, More, Karren L., Lupini, Andrew, Allard, Lawrence F., Markovic, Nenad M., and Stamenkovic, Vojislav R. Wed .
"Surface faceting and elemental diffusion behaviour at atomic scale for alloy nanoparticles during in situ annealing". United States. https://doi.org/10.1038/ncomms9925. https://www.osti.gov/servlets/purl/1249113.
@article{osti_1249113,
title = {Surface faceting and elemental diffusion behaviour at atomic scale for alloy nanoparticles during in situ annealing},
author = {Chi, Miaofang and Wang, Chao and Lei, Yinkai and Wang, Guofeng and Li, Dongguo and More, Karren L. and Lupini, Andrew and Allard, Lawrence F. and Markovic, Nenad M. and Stamenkovic, Vojislav R.},
abstractNote = {The catalytic performance of nanoparticles is primarily determined by the precise nature of the surface and near-surface atomic configurations, which can be tailored by post-synthesis annealing effectively and straightforwardly. Understanding the complete dynamic response of surface structure and chemistry to thermal treatments at the atomic scale is imperative for the rational design of catalyst nanoparticles. Here, by tracking the same individual Pt3Co nanoparticles during in situ annealing in a scanning transmission electron microscope, we directly discern five distinct stages of surface elemental rearrangements in Pt3Co nanoparticles at the atomic scale: initial random (alloy) elemental distribution; surface platinum-skin-layer formation; nucleation of structurally ordered domains; ordered framework development and, finally, initiation of amorphization. Furthermore, a comprehensive interplay among phase evolution, surface faceting and elemental inter-diffusion is revealed, and supported by atomistic simulations. In conlcusion, this work may pave the way towards designing catalysts through post-synthesis annealing for optimized catalytic performance.},
doi = {10.1038/ncomms9925},
journal = {Nature Communications},
number = 8925,
volume = 6,
place = {United States},
year = {Wed Nov 18 00:00:00 EST 2015},
month = {Wed Nov 18 00:00:00 EST 2015}
}
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