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Title: Quantitative 3D evolution of colloidal nanoparticle oxidation in solution

Abstract

Real-time tracking three-dimensional (3D) evolution of colloidal nanoparticles in solution is essential for understanding complex mechanisms involved in nanoparticle growth and transformation. We simultaneously use time-resolved small-angle and wide-angle x-ray scattering to monitor oxidation of highly uniform colloidal iron nanoparticles, enabling the reconstruction of intermediate 3D morphologies of the nanoparticles with a spatial resolution of ~5 Å. The in-situ probing combined with large-scale reactive molecular dynamics simulations reveals the transformational details from the solid metal nanoparticles to hollow metal oxide nanoshells via nanoscale Kirkendall process, for example, coalescence of voids upon their growth, reversing of mass diffusion direction depending on crystallinity, and so forth. In conclusion, our results highlight the complex interplay between defect chemistry and defect dynamics in determining nanoparticle transformation and formation.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [3]; ORCiD logo [3];  [3]
  1. Department of Chemistry, Temple University, 1901 North 13th Street, Philadelphia, PA 19122, USA.
  2. X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439, USA.
  3. Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439, USA.
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1436809
Alternate Identifier(s):
OSTI ID: 1374052
Grant/Contract Number:  
award303569; AC02-05CH11231; award303568; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 356 Journal Issue: 6335; Journal ID: ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; SAXS; nanoparticle

Citation Formats

Sun, Yugang, Zuo, Xiaobing, Sankaranarayanan, Subramanian K. R. S., Peng, Sheng, Narayanan, Badri, and Kamath, Ganesh. Quantitative 3D evolution of colloidal nanoparticle oxidation in solution. United States: N. p., 2017. Web. doi:10.1126/science.aaf6792.
Sun, Yugang, Zuo, Xiaobing, Sankaranarayanan, Subramanian K. R. S., Peng, Sheng, Narayanan, Badri, & Kamath, Ganesh. Quantitative 3D evolution of colloidal nanoparticle oxidation in solution. United States. https://doi.org/10.1126/science.aaf6792
Sun, Yugang, Zuo, Xiaobing, Sankaranarayanan, Subramanian K. R. S., Peng, Sheng, Narayanan, Badri, and Kamath, Ganesh. Fri . "Quantitative 3D evolution of colloidal nanoparticle oxidation in solution". United States. https://doi.org/10.1126/science.aaf6792.
@article{osti_1436809,
title = {Quantitative 3D evolution of colloidal nanoparticle oxidation in solution},
author = {Sun, Yugang and Zuo, Xiaobing and Sankaranarayanan, Subramanian K. R. S. and Peng, Sheng and Narayanan, Badri and Kamath, Ganesh},
abstractNote = {Real-time tracking three-dimensional (3D) evolution of colloidal nanoparticles in solution is essential for understanding complex mechanisms involved in nanoparticle growth and transformation. We simultaneously use time-resolved small-angle and wide-angle x-ray scattering to monitor oxidation of highly uniform colloidal iron nanoparticles, enabling the reconstruction of intermediate 3D morphologies of the nanoparticles with a spatial resolution of ~5 Å. The in-situ probing combined with large-scale reactive molecular dynamics simulations reveals the transformational details from the solid metal nanoparticles to hollow metal oxide nanoshells via nanoscale Kirkendall process, for example, coalescence of voids upon their growth, reversing of mass diffusion direction depending on crystallinity, and so forth. In conclusion, our results highlight the complex interplay between defect chemistry and defect dynamics in determining nanoparticle transformation and formation.},
doi = {10.1126/science.aaf6792},
journal = {Science},
number = 6335,
volume = 356,
place = {United States},
year = {Fri Apr 21 00:00:00 EDT 2017},
month = {Fri Apr 21 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1126/science.aaf6792

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Cited by: 109 works
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