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@ARTICLE{Huittinen:845786,
author = {Huittinen, Nina and Scheinost, Andreas C. and Ji, Yaqi and
Kowalski, Piotr and Arinicheva, Yulia and Wilden, Andreas
and Neumeier, Stefan and Stumpf, Thorsten},
title = {{A} {S}pectroscopic and {C}omputational {S}tudy of {C}m 3+
{I}ncorporation in {L}anthanide {P}hosphate {R}habdophane
({L}n{PO} 4 ·0.67{H}2{O}) and {M}onazite ({L}n{PO}4 )},
journal = {Inorganic chemistry},
volume = {57},
number = {11},
issn = {1520-510X},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2018-02993},
pages = {6252–6265},
year = {2018},
abstract = {This study investigates the incorporation of the minor
actinide curium (Cm3+) in a series of synthetic La1-xGdxPO4
(x = 0, 0.24, 0.54, 0.83, 1) monazite and rhabdophane solid
solutions. To obtain information of the incorporation
process on the molecular scale and to understand the
distribution of the dopant in the synthetic phosphate
phases, combined time-resolved laser fluorescence
spectroscopy (TRLFS) and x-ray absorption fine structure
(XAFS) spectroscopy investigations have been conducted and
complemented with ab initio atomistic simulations. We found
that Cm3+ is incorporated in the monazite endmembers (LaPO4
and GdPO4) on one specific, highly ordered lattice site. The
intermediate solid solutions, however, display increasing
disorder around the Cm3+ dopant as a result of random
variations in nearest neighbor distances. In hydrated
rhabdophane, and especially its La-rich solid solutions,
Cm3+ is preferentially incorporated on non-hydrated lattice
sites. This site occupancy is not in agreement with the
hydrated rhabdophane structure, where two thirds of the
lattice sites are associated with water of hydration
(LnPO4·0.67H2O), implying that structural substitution
reactions cannot be predicted based on the structure of the
host matrix only.},
cin = {IEK-6 / IEK-1 / JARA-HPC},
ddc = {540},
cid = {I:(DE-Juel1)IEK-6-20101013 / I:(DE-Juel1)IEK-1-20101013 /
$I:(DE-82)080012_20140620$},
pnm = {161 - Nuclear Waste Management (POF3-161) / BMBF-02NUK021A
- Verbundprojekt Conditioning: Grundlegende Untersuchungen
zur Immobilisierung langlebiger Radionuklide mittels Einbau
in endlagerrelevante Keramiken; Teilprojekt A
(BMBF-02NUK021A) / Atomistic modeling of
radionuclide-bearing materials for safe management of high
level nuclear waste. $(jara0037_20181101)$ / Investigation
of the new materials for safe management of high level
nuclear waste. $(jara0038_20121101)$ / Investigation of the
new materials for safe management of high level nuclear
waste. $(jiek61_20131101)$},
pid = {G:(DE-HGF)POF3-161 / G:(DE-Juel1)BMBF-02NUK021A /
$G:(DE-Juel1)jara0037_20181101$ /
$G:(DE-Juel1)jara0038_20121101$ /
$G:(DE-Juel1)jiek61_20131101$},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:29762025},
UT = {WOS:000434491700012},
doi = {10.1021/acs.inorgchem.8b00095},
url = {https://juser.fz-juelich.de/record/845786},
}