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Issue 18, 2020
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Structural properties of ultra-small thorium and uranium dioxide nanoparticles embedded in a covalent organic framework

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Abstract

We report the structural properties of ultra-small ThO2 and UO2 nanoparticles (NPs), which were synthesized without strong binding surface ligands by employing a covalent organic framework (COF-5) as an inert template. The resultant NPs were used to observe how structural properties are affected by decreasing grain size within bulk actinide oxides, which has implications for understanding the behavior of nuclear fuel materials. Through a comprehensive characterization strategy, we gain insight regarding how structure at the NP surface differs from the interior. Characterization using electron microscopy and small-angle X-ray scattering indicates that growth of the ThO2 and UO2 NPs was confined by the pores of the COF template, resulting in sub-3 nm particles. X-ray absorption fine structure spectroscopy results indicate that the NPs are best described as ThO2 and UO2 materials with unpassivated surfaces. The surface layers of these particles compensate for high surface energy by exhibiting a broader distribution of Th–O and U–O bond distances despite retaining average bond lengths that are characteristic of bulk ThO2 and UO2. The combined synthesis and physical characterization efforts provide a detailed picture of actinide oxide structure at the nanoscale, which remains highly underexplored compared to transition metal counterparts.

Graphical abstract: Structural properties of ultra-small thorium and uranium dioxide nanoparticles embedded in a covalent organic framework

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Article information


Submitted
04 Dec 2019
Accepted
13 Apr 2020
First published
28 Apr 2020

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020,11, 4648-4668
Article type
Edge Article

Structural properties of ultra-small thorium and uranium dioxide nanoparticles embedded in a covalent organic framework

L. M. Moreau, A. Herve, M. D. Straub, D. R. Russo, R. J. Abergel, S. Alayoglu, J. Arnold, A. Braun, G. J. P. Deblonde, Y. Liu, T. D. Lohrey, D. T. Olive, Y. Qiao, J. A. Rees, D. K. Shuh, S. J. Teat, C. H. Booth and S. G. Minasian, Chem. Sci., 2020, 11, 4648 DOI: 10.1039/C9SC06117G

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