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@PHDTHESIS{Sun:890450,
author = {Sun, Yajie},
title = {{U}ranium accumulation in agricultural soilsas derived from
long-term phosphorus fertilizer applications},
volume = {527},
school = {Universität Bonn},
type = {Dr.},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2021-00966},
isbn = {978-3-95806-521-5},
series = {Schriften des Forschungszentrums Jülich. Reihe Energie
$\&$ Umwelt / Energy $\&$ Environment},
pages = {XII, 136 S.},
year = {2020},
note = {Universität Bonn, Diss., 2020},
abstract = {It is well known that uranium (U) in mineral phosphorus (P)
fertilizers may accumulate in agricultural soils; yet, this
U accumulation occurs at different rates, likely depending
on the type of fertilizer used. To substantiate this
assumption, the aims of my thesis were: i) to quantify the
accumulation rates of fertilizer-derived U in different
long-term agricultural field experiments with P fertilized
soils of central Europe, and ii) to contrast this with data
from longterm experimental sites on volcanic soils that
require higher amounts of P fertilizers for optimal crop
production, and iii) finally to explain the variations of U
accumulation rates by an assessment of the formation
mechanisms and stocks of U in major phosphate rocks (PRs)
deposits of the world. Soil samples were taken from the
surface soils and selected depth profiles of seven long-term
experiment sites, i.e. at the grassland fertilization trials
in Rengen (Germany), Park Grass (Rothamsted, UK), as well as
in Geitasandur and Sámstaðir (Iceland), and the
agricultural field experimental sites in Thyrow (Germany),
Askov (Denmark), Broadbalk (Rothamsted, UK), Uranium
concentrations were analyzed after microwave-assisted acid
digestion by nitric acidor/and a complete digestion by
lithium meta/tetraborate. In addition, I assessed U
concentrations and the natural stable oxygen isotope
compositions of phosphate (δ$^{18}$OP) in PRs as potential
indicators for the genesis of the U in PRs from different
deposits all over the world. My results revealed a wide
range of U accumulation rates in soils, ranging from 0-310
μg U kg$^{-1}$ yr$^{-1}$ in the monitored fields. Uranium
accumulation was small when the P fertilizers were derived
from igneous PRs from Finland and Kola Peninsula, as used
for sites in Askov (< 0.4 μg U kg$^{-1}$ yr$^{-1}$; <1.2 g
ha$^{-1}$ yr$^{-1}$ (20 cm)) and Thyrow (0.6 μg U kg$^{-1}$
yr$^{-1}$; 2.3 g ha$^{-1}$ yr$^{-1}$ (24 cm)), respectively,
or when basic slag was applied as used for the Rengen (1.2
μg U kg$^{-1}$ yr$^{-1}$; 1.3 g ha$^{-1}$ yr$^{-1}$ (10
cm)) site. Higher U accumulation rates (3.4, 7.8 μg U
kg$^{-1}$ yr$^{-1}$; 11.7, 21.9 g ha$^{-1}$ yr$^{-1}$ (23
cm)) were found at Rothemsted experiment stations
(Broadbalk; Parkgrass), where P fertilizers used had been
predominantly produced from PRs from North Africa. The most
serious case of fertilizer-derived U accumulation (up to 310
μg U kg$^{-1}$ yr$^{-1}$; 33.2 g ha$^{-1}$ yr$^{-1}$ (5
cm)) was found in Icelandic agricultural soil as a
consequence of both high U concentrations in the applied P
fertilizers (from an unknown PR source) and of large amounts
of P fertilizer application. Overall, soil U concentrations
will increase by 0.5 μg U kg$^{-1}$ (0-5.1 μg U kg$^{-1}$)
soil for 1 kg P applied per hectare and there will be 2.7-11
g U ha$^{-1}$ yr$^{-1}$ input to the EU’s agricultural
soil with 21.2 kg P (as P$_{2}$O$_{5}$) per hectare
fertilization. To explain these variations of U
concentrations in the world’s PRs, U concentrations in the
PRs were discussed corresponding to their δ$^{18}$OP
values. I found that there was a ‘coevolutionary’
relationship between the U (U/P$_{2}$O$_{5}$ ratio) and the
δ$^{18}$OP value: the lower the δ$^{18}$Op value of the PR
was, the lower its U concentration was. In igneous PRs, low
U concentration can be explained by the lack of secondary U
enrichment processes after rock formation, whereas the low
δ$^{18}$Op values was resulted from limited isotope
fractionation at high temperatures in the magma. In
sedimentary PRs, on the other hand, the variations of U
concentrations and δ$^{18}$Op values were related to the
geologic age at which PRs were formed. Generally, older
sedimentary PRs (formed in Precambrian-Cambrian) exhibited
lower U concentrations and lower δ$^{18}$Op values than the
younger ones (formed in Ordovician-Neogene), which were
influenced by paleoclimate and paleographic features. In
summary, the accumulation rates of fertilizer-derived U in
agricultural soils were regionspecific, depending on the
source and the amount of P fertilizer applied. My data show
that when applying P fertilizers with low U content, soil U
concentration will remain at a non-critical level even at
multi-centennial scale. However, fertilizer-derived U
accumulation may pose an environmental issue at the places
where large amounts of P fertilizers are needed for
maximizing crop production (such as in Andosols). Selecting
igneous PRs or ancient sedimentary PRs (formed in Paleozoic
and Precambrian) as precursor materials for P fertilizer
production is therefore crucial for minimizing potential U
contamination risks and thus for sustainable agricultural
management.},
cin = {IBG-3},
cid = {I:(DE-Juel1)IBG-3-20101118},
pnm = {255 - Terrestrial Systems: From Observation to Prediction
(POF3-255)},
pid = {G:(DE-HGF)POF3-255},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
url = {https://juser.fz-juelich.de/record/890450},
}