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

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 [2] ;  [2] ; ORCiD logo [2] ;  [2]
  1. Temple Univ., Philadelphia, PA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 356; Journal Issue: 6335; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; SAXS; nanoparticle
OSTI Identifier:
1374052

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., 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. doi:10.1126/science.aaf6792.
Sun, Yugang, Zuo, Xiaobing, Sankaranarayanan, Subramanian K. R. S., Peng, Sheng, Narayanan, Badri, and Kamath, Ganesh. 2017. "Quantitative 3D evolution of colloidal nanoparticle oxidation in solution". United States. doi:10.1126/science.aaf6792. https://www.osti.gov/servlets/purl/1374052.
@article{osti_1374052,
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 = {2017},
month = {4}
}

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