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Quantitative 3D evolution of colloidal nanoparticle oxidation in solution

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Science  21 Apr 2017:
Vol. 356, Issue 6335, pp. 303-307
DOI: 10.1126/science.aaf6792

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Watching nanomaterials transform in time

Real-time analysis of chemical transformations of nanoparticles is usually done with electron microscopy of a few particles. One limitation is interference by the electron beam. Sun et al. monitored the oxidation of iron nanoparticles in solution by using small- and wide-angle x-ray scattering and molecular dynamics simulations (see the Perspective by Cadavid and Cabot). These methods revealed the formation of voids within the nanoparticles, diffusion of material into and out of the nanoparticles, and ultimately the coalescence of the voids.

Science, this issue p. 303; see also p. 245

Abstract

Real-time tracking of the three-dimensional (3D) evolution of colloidal nanoparticles in solution is essential for understanding complex mechanisms involved in nanoparticle growth and transformation. We used time-resolved small-angle and wide-angle x-ray scattering simultaneously 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 angstroms. The in situ observations, combined with large-scale reactive molecular dynamics simulations, reveal the details of the transformation from solid metal nanoparticles to hollow metal oxide nanoshells via a nanoscale Kirkendall process—for example, coalescence of voids as they grow and reversal of mass diffusion direction depending on crystallinity. Our results highlight the complex interplay between defect chemistry and defect dynamics in determining nanoparticle transformation and formation.

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