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@ARTICLE{Arinicheva:849928,
author = {Arinicheva, Yulia and Gausse, Clemence and Neumeier, Stefan
and Brandt, Felix and Rozov, Konstantin and Szenknect,
Stéphanie and Dacheux, Nicolas and Bosbach, Dirk and
Deissmann, Guido},
title = {{I}nfluence of temperature on the dissolution kinetics of
synthetic {L}a{PO}4-monazite in acidic media between 50 and
130 °{C}},
journal = {Journal of nuclear materials},
volume = {509},
issn = {0022-3115},
address = {Amsterdam [u.a.]},
publisher = {Elsevier Science},
reportid = {FZJ-2018-04024},
pages = {488-495},
year = {2018},
abstract = {Single-phase monazite-type ceramics are discussed as waste
forms for the safe disposal of surplus plutonium or
separated minor actinides. To gain a deeper insight into the
mechanism governing the dissolution of monazite-type
compounds, the dissolution kinetics of synthetic
LaPO4-monazite was systematically studied by dynamic
dissolution experiments carried out in the temperature range
from 50 to 130 °C in acidic media (0.01 M HNO3). The
dissolution rates at far from equilibrium conditions
increased from 3.2 × 10−5 g m−2 d−1 at
50 °C to 2.5 × 10−4 g m−2 d−1 at
130 °C. Two different temperature regions were observed,
in which the normalised dissolution rates of LaPO4 have a
diverging temperature dependence, indicating two different
mechanisms of dissolution: namely surface-controlled
dissolution (T = 50–90 °C;
Ea = 44 kJ mol−1) and transport-controlled
dissolution (T = 90–130 °C;
Ea = 7.5 kJ mol−1). Complementary thermodynamic
modelling studies of the dissolution of LaPO4 at the
experimental conditions show that La-rhabdophane
(LaPO4·0.667H2O) is the thermodynamically favoured
phosphate phase in aqueous environments below about
100 °C. Apparently, the hydration of monazite and the
formation of a thin surface layer consisting of rhabdophane
is an intermediate step controlling the dissolution kinetics
of the LaPO4 monazite ceramics in low temperature aqueous
environments.Keywords},
cin = {IEK-6 / IEK-1},
ddc = {530},
cid = {I:(DE-Juel1)IEK-6-20101013 / I:(DE-Juel1)IEK-1-20101013},
pnm = {161 - Nuclear Waste Management (POF3-161)},
pid = {G:(DE-HGF)POF3-161},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000442483300054},
doi = {10.1016/j.jnucmat.2018.07.009},
url = {https://juser.fz-juelich.de/record/849928},
}