Quantitative 3D evolution of colloidal nanoparticle oxidation in solution

Sun, Yugang; Zuo, Xiaobing; Sankaranarayanan, Subramanian K. R. S.; Peng, Sheng; Narayanan, Badri; Kamath, Ganesh

doi:10.1126/science.aaf6792

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

Journal Article · Fri Apr 21 00:00:00 EDT 2017 · Science

DOI:https://doi.org/10.1126/science.aaf6792· OSTI ID:1436809

^[1];

^[2];

^[3]; Peng, Sheng ^[3];

^[3]; Kamath, Ganesh ^[3]

Department of Chemistry, Temple University, 1901 North 13th Street, Philadelphia, PA 19122, USA.
X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439, USA.
Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439, USA.

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: award303569; AC02-05CH11231; award303568; AC02-06CH11357

OSTI ID:: 1436809

Alternate ID(s):: OSTI ID: 1374052

Journal Information:: Science, Journal Name: Science Vol. 356 Journal Issue: 6335; ISSN 0036-8075

Publisher:: American Association for the Advancement of Science (AAAS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 109 works

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