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@ARTICLE{Finkeldei:873032,
author = {Finkeldei, S. and Stennett, M. C. and Kowalski, P. M. and
Ji, Y. and de Visser-Týnová, E. and Hyatt, N. C. and
Bosbach, D. and Brandt, F.},
title = {{I}nsights into the fabrication and structure of plutonium
pyrochlores},
journal = {Journal of materials chemistry / A Materials for energy and
sustainability A},
volume = {8},
number = {5},
issn = {2050-7496},
address = {London [u.a.]},
publisher = {RSC},
reportid = {FZJ-2020-00483},
pages = {2387-2403},
year = {2020},
abstract = {Rare earth zirconates, such as Nd2Zr2O7, crystallise with
the pyrochlore structure and are a group of materials which
have been suggested as potential nuclear waste forms for
actinide immobilisation. In this work, a new hydroxide
co-precipitation route is presented to investigate the
incorporation of Pu into Nd2Zr2O7. The plutonium content was
varied between 5 and 10 $mol\%$ and the structural uptake
and Pu oxidation state were probed by X-ray diffraction
(XRD), scanning electron microscopy (SEM), and X-ray
absorption spectroscopy (XAS). The experimental findings
were complemented by DFT ab initio calculations. For all the
incorporation mechanisms studied PuO2 was used as the
reference reactant state to allow for a direct comparison
between the possible Pu uptake scenarios. Analysis of the
experimental data suggests that Pu(IV) cations substitute
for Nd(III) cations leading to structural distortion of the
pyrochlore A-sites. The computed solution energies and
bond-distances corroborate the experimental findings and
indicate that the excess charge is balanced via the
introduction of oxygen at formerly vacant sites.},
cin = {IEK-6 / JARA-HPC},
ddc = {530},
cid = {I:(DE-Juel1)IEK-6-20101013 / $I:(DE-82)080012_20140620$},
pnm = {161 - Nuclear Waste Management (POF3-161) / Investigation
of the new materials for safe management of high level
nuclear waste. $(jara0038_20121101)$},
pid = {G:(DE-HGF)POF3-161 / $G:(DE-Juel1)jara0038_20121101$},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000521200000063},
doi = {10.1039/C9TA05795A},
url = {https://juser.fz-juelich.de/record/873032},
}