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Transfer of natural radionuclides from soils to plants in a marsh enhanced by the operation of non-nuclear industries

Abstract

Two sampling campaigns were performed in 1993 at the marsh area (Odiel marsh) located in southwestern Spain, in the city of Huelva. Spartina densiflora and substrate soil (5 cm deep) samples were collected in several locations across the area in each campaign. Activity concentrations of 210Po, U-and Th-isotopes were determined in the plant and the substrate samples. The production of phosphoric acid from phosphate mineral in the vicinity clearly enhances the concentrations of these radionuclides in certain areas of the marsh. Moreover, concentrations in plants are affected by the concentration of the same element in its substrate. Indeed, high concentration levels in plants are coincident with high concentration in soils. However, concentration ratios (CR), defined as the ratio between the concentration of an element in the plant and of that in its substrate, are higher when substrate concentrations are low, whereas low CR values are found in areas where substrate concentrations are high. Moreover, both variables (CR and soil concentration) seem to be non-linearly related, at least, in the case of radionuclides from the 238U decay chain.

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Transfer of natural radionuclides from soils to plants in a marsh enhanced by the operation of non-nuclear industries

Author: Martínez Aguirre, Aránzazu; García Orellana, Isabel; García León, Manuel
Publisher: Elsevier
Year: 1997
DOI: 10.1016/S0265-931X(96)00048-3
Source: https://idus.us.es/bitstreams/959b21b9-2ece-4a68-9544-323fd24fd047/download
T ans e o Na u al Radionuclides om Soils o Plan s in
a Ma sh Enhanced by he Ope a ion o Non-Nuclea
Indus ies
A. Ma ínez-Agui e/ l. Ga cía-O ellanab & M. Ga cía-Leónb
ªDep. Física Aplicada, EUITA, Uni e sidad de Se illa, Ca e e a U e a, km 1,
41080 Se illa, Spaín
bFacul ad de Física, Uni e sidad de Se illa, Apdo 1065, 41080 Se illa, Spain
ABSTRACT
Two sampling campaigns we e pe o med in 1993 a he ma sh a ea (Odie/
ma sh) loca ed in sou hwes e n Spain, in he ci y o Huel a. Spa ina densi
lo a and subs a e soil ( 5 cm deep) samples we e collec ed in se e a/ loca
ions ac oss he a ea in each campaign. Ac i i y concen a ions o 210Po, U
and Th-iso opes we e de e mined in he plan and he subs a e samples. The
p oduc ion o phospho ic acid om phospha e mine al in he icini y clea ly
enhances he concen a ions o hese adionuclides in ce ain a eas o he
ma sh. Mo eo e , concen a ions in plan s a e a ec ed by he concen a ion
o he same elemen in i s subs a e. Indeed, high concen a ion le els in
plan s a e coinciden wi h high concen a ion in soils. Howe e , concen a ion
a ios ( CR), de ined as he a io be ween he concen a ion o an elemen in
he plan and o ha in i s subs a e, a e highe when subs a e concen a ions
a e low, whe eas low CR alues a e ound in a eas whe e subs a e concen
a ions a e high. Mo eo e , bo h a iables (CR and soil concen a ion)
seem o be non-linea /y ela ed, a leas , in he case o adionuclides om he
238U decay chain.
INTRODUCTION
En i onmen al assessmen s use ood-chain models o de e mine he <lose
o man om adionuclides eleased o he biosphe e. T adi ional ood
chain models equi e a plan /subs a e ans e coe icien , e e ed o as a
concen a ion a io (CR). The concen a ion a io o ans e coe icien
concep , is gene ally accep ed and widely used in en i onmen al anspo
models and desc ibes he amoun s o nuclide expec ed o en e a plan
om i s subs a e.
The CR app oach equi es us o assume ha he plan and subs a e
concen a ions a e linea ly ela ed and ha he line de ining he ela ion
ship goes h ough he o igin. The a iabili y o CR has p e iously been
add essed, bu ew ha e speci ically add essed he linea i y assump ion.
This assump ion implies ha , unde compa able condi ions, he CR o an
elemen is cons an , ega dless o subs a e concen a ion (Sheppa d &
Sheppa d, 1985).
Howe e , plan up ake o elemen s, bo h essen ial and non-essen ial o
g ow h, di e s and may ollow a non-linea ela ionship. Cannon (1952)
has s a ed ha U may be a mic onu ien o highe plan s, which means
ha CR was no linea ly ela ed o he subs a e concen a ion.
Mo dbe g e al. (1976) ob ained CR alues by i ing linea and
hype bolic unc ions o da a ob ained using di e en soil concen a ions
o iso opes in he U-Ra se ies. They showed ha he CR was cons an
o e hei obse ed soil concen a ions. Cannon (1952) also sugges ed a
linea ela ionship exis ing o U be ween plan and soil concen a ions.
Howe e , Mo ishima e al. (1976) epo ed a non-linea ela ionship o
U be ween ege able and soil concen a ions. Lopa kina e al. (1970)
ha e sugges ed ha he linea i y assump ion may hold only o p imi i e
plan o ms. Sheppa d and Sheppa d ( 1985) s udied he linea i y
assump ion o U in plan s and subs a e a wo o e bodies on he
P ecamb ian Shield. They ound ha he ela ionship be ween CR and
subs a e concen a ion obse ed in na i e plan s ends o be hype bolic,
wi h a endency o CR alues o be la ge a lowe subs a e concen
a ions. I appea s, he e o e, ha U may beha e as an essen ial
elemen a low subs a e concen a ions. Many da a sugges ha plan
concen a ions a e un ela ed o soil concen a ions, and when a line is
i ed o he da a, he in e cep is usually g ea e han ze o (Simon &
lb ahim, 1987). Log-no mal dis ibu ions o concen a ion a ios we e
epo ed by Sheppa d and E enden (1988). They p oposed ha he
linea i y assump ion, al hough con a y o wha is usually expec ed o
nu ien s (essen ial) elemen s, may be alid o limi ed anges o soil
concen a ions o o elemen s no physiologically egula ed by plan s.
Many expe imen s designed o measu e CR alues ha e used only a ew
di e en soil concen a ions and hus, canno s a is ically assess he
linea i y assump ion. Simon and Ib ahim (1987) p oposed ha a cu i
linea ela ionship e lec ing a sa u a ion- ype mechanism in plan s was
mo e app op ia e.
A hypo he ical ela ionship o he CR o essen ial and non-essen ial
elemen s o e a ange o subs a e concen a ions is shown in Fig. 1. This
ela ionship means ha plan s eadily ake up elemen s essen ial o plan
g ow h when subs a e concen a ions a e low, whe eas plan up ake o
non-essen ial elemen s is gene ally cons an in his subs a e concen a ion
ange (Timpe ley e al., 1970; Mengel & Ki kby, 1979). A high subs a e
concen a ions, plan up ake o essen ial and non-essen ial elemen s can
ei he be cons an (no oxici y) o can dec ease, leading o oxici y o
dea h. Toxici y begins a a oxici y h eshold, he subs a e concen a ion
a which plan g ow h, and hence up ake, begin o be impai ed. Le hal
subs a e concen a ions o an essen ial o non-essen ial elemen may no
exis , and in ha case, he CR may be cons an o se e a} o de s o
magni ude.
The CR concep is CR = Cp/Cs = cons an , and i is p obably use ul o
non-essen ial elemen s a non- oxic subs a e le els. The lack o co ela
ion be ween plan and subs a e concen a ions o non-essen ial elemen s
could be explained i he elemen is mimicking an essen ial elemen
(Sheppa d & Sheppa d, 1985). This ac would esul in a non-linea ela
ionship be ween he CR and he subs a e concen a ion a low subs a e
concen a ion. This ela ionship could be modelled as:
De icien To!e an
Non Essen iol-
Soil Concen o ion
Toxic
...
Toxici y
Th es íold
Non- oxic
/Le hal
(1)
Fig. l. Hypo he ical ela ionship o CR s soil concen a ion o bo h essen ial and non
essen ial elemen s h ough he de icien o oxic soil-concen a ion ange (Sheppa d &
Sheppa d, 1985).
whe e Cp is he concen a ion in he plan and Cs is he concen a ion in
he subs a e. This esul s in:
Cp a
CR =Cs
= Cs +b. (2)
I he i s ela ionship does no ha e a ze o in e cep (a i-O), his
would mean ha CR (Cp/Cs) is dependen on he subs a e concen a ion.
T acy e al. (1983) s udied he up ake o
226Ra, 21°I>b and U om soils o
ga den p oduce. They obse ed a clea end o inc easing concen a ions in
plan s wi h inc easing concen a ion in soil subs a e. In o de o exp ess
his end quan i a i ely, a linea eg ession analysis was ca ied ou o he
loga i hms o he mean ege able concen a ion s he loga i hms o he soil
concen a ions. This in ol es i ing a unc ion o he o m:
o
CR = acb-i
s '
whe e a and b a e pa ame e s o be de e mined.
(3)
(4)
A alue o b equal o 1.00 would imply a linea ela ionship (CR = Cp/
Cs = c e). They ound ha hei esul s we e no inconsis en wi h he line
a i y assump ion, a leas o concen a ions up o abou 37 Bq g-1 in soil.
The use o concen a ion a ios o p edic plan concen a ions om
low subs a e concen a ion o en i onmen al assessmen pu poses
should be in es iga ed u he o adionuclides known o mimic essen ial
elemen s and should be measu ed unde na u al condi ions (Sheppa d &
Sheppa d, 1985).
This pape e eals a s udy o he dis ibu ion and ans e o
210Po-, U
and Th-iso opes om soils o Spa ina densi lo a (a wild plan species
ypical o ma sh a eas in Eu ope) collec ed om a saline ma sh loca ed in
sou hwes Spain. The p esence, in he icini y, o a e ilize complex
which uses mine al wi h high U concen a ion could allow o a wide soil
concen a ion ange in he s udied a ea (Ma ínez-Agui e & Ga cía
León, 1997). Indeed, he main aim o he wo k is o con ibu e a bi mo e
in he s udy abou how na u al adionuclides a e being inco po a ed in he
plan om i s subs a e concen a ion. Thus, a s udy o he CR ela ion
ship wi h he concen a ion in he soil subs a e will ollow. Al hough his
species is no di ec ly in ol ed in he human ood chain, in o ma ion on
he concen a ion le els and ans e o adionuclides om con amina ed
soils will p o ide impo an da a on he ans e mechanisms in he case o
hose species mo e di ec ly in ol ed in he human die .
SAMPLES AND RADIOANAL YTICAL PROCEDURES
Se e al s a ions we e chosen ac oss he Odiel ma sh a ea o Huel a o
sample collec ion. This a ea is clea ly a ec ed by he was es eleased by
wo e ilize ac o ies loca ed in he icini y (see Fig. 2). The a ea is
cons i u ed by ou small islands sepa a ed by ou channels, which a e
a ec ed, due o idal mo emen s, by he in low o he Odiel i e wa e s
(Ma ínez-Agui e & Ga cía-León, 1997). Samples (plan and subs a e)
we e collec ed, du ing he low ide, a he bo de o he channels, in a eas
co e ed wi h wa e du ing he high ide.
A lan :c Ocean
Huel a
Town
Fig. 2. Loca ion o he sampling s a ions in he Odie! ma sh a ea. The loca ions o he
e ilize complex and he phosphogypsum piles a e also gi en.

Abou 1 kg o soil sample was collec ed om each s a ion and s o ed in
plas ic bags. A he labo a o y, hey we e d ied and powde ed be o e he
adionuclide analysis. The bulk d y densi y (g cm -3) and pe cen age o
o ganic ma e we e de e mined in each soil sample. Spa ina densi lo a
samples we e collec ed a he same s a ions and a he same ime as soil
samples. The oo s o he plan s we e sepa a ed in o de o s udy only he
o e g ound pa o he plan s. Once sepa a ed, he samples we e washed
wi h wa e o emo e any ace o solid pa icles. Finally, hey we e ai 
d ied and powde ed o analysis.
Aliquo s o each sample (soil and/o plan ) we e used o Po- and U
and Th-iso opes de e mina ions, sepa a ely. They we e diges ed wi h
concen a ed HN03 and aqua egia and he inal esidue dissol ed in 8M
HN03. Be o e he diges ion, he samples we e spiked wi h known
amoun s o 208Po ac i i ies o 210Po de e mina ion, and o 232U and 229Th
ac i i ies o U and Th iso opes de e mina ions, sepa a ely. Polonium-210
was sepa a ed om ac inides by a sol en ex ac ion me hod which used
TBP ( ibu ylphospha e) as he ex ac an phase. Polonium emained in
he ni ic phase, whe eas ac inides mo ed o he o ganic (TBP) phase
(Ma ínez-Agui e, 1991). The inal Po solu ion was e apo a ed and sel 
deposi ed on o 2.2 cm diame e sil e planche s. Polonium ac i i ies we e
de e mined by .(-spec ome y wi h ion-implan ed de ec o s.
Fo U- and Th-iso ope de e mina ions, an ion-exchange me hod was
used. A e edissolu ion o he esidue wi h 8M HN03, p ecipi a ion o
i on hyd oxides was ca ied ou by adding concen a ed ammonium.
U anium- and Th-iso opes we e sepa a ed and pu i ied in a DOWEX
AG1-X8 (chlo ide o m) esin (Ma ínez-Agui e, 1991). Final solu ions
we e elec opla ed on o 2.2-cm diame e s ainless s eel planche s, sepa
a ely. U anium- and Th-iso opes ac i i ies we e also de e mined by .(
spec ome y wi h ion-implan ed de ec o s.
RESULTS AND DISCUSSION
In Tables 1 and 2, da a on 210Po-, U- and Th-iso opes in soils and Spa ina
densi lo a o each sampling s a ion a e gi en, espec i ely. Table 1 also
includes he pe cen age o o ganic ma e in each soil sample. Mo eo e ,
in Table 3, concen a ion a ios (CR), de ined as he concen a ion o an
elemen in he plan (mBq g-1 d y weigh ) di ided by he concen a ion o
he same elemen in he subs a e (mBq g-1 d y weigh ), a e also gi en.
The nex sec ions discuss sepa a ely, da a on soil and plan concen a ions
and, inally, he CR esul s.
Soil subs a e
In gene al, by conside ing he le els o all adionuclides om he 238U
decay chain, a easonably wide ange o ac i i y concen a ion in he soil
samples, is ound. The e a e samples wi h low concen a ions o
238U and
descendan s, which can be conside ed as clea ly non-enhanced by he
e ilize indus ies. In gene al, concen a ion le els in hese samples a e
below 70 mBq g-1, le els simila o hose ypical in undis u bed soils
( anging om 10 o 50mBqg-1, UNSCEAR, 1988). These samples we e
collec ed in s a ions u he away om he e ilize indus ies, in he wes
pa o he Sal és island along he Pun a Umb ia i e . Also, e y low
concen a ion le els we e ound in wo s a ions a he eas side o he
Bacu a island opposi e he e ilize indus ies. This ac mus be ela ed o
he composi ion o he sample. Indeed, alues o densi y and o ganic
ma e (see Table 1) in bo h samples e lec ha high amoun s o sandy
pa icles, wi h low ac i i y concen a ions, a e con ained in such samples.
So ne o he samples e eal in e media e concen a ion le els (clea ly
highe han backg ound, bu no e y high) o all adionuclides om he
238U decay chain, anging om abou 100 o 300 mBq g-1. These samples
a e loca ed along he eas pa o he Enmedio island and he wes pa o he
Bacu a island, washed by he Moja e a channel. Finally, he e a e samples
wi h much highe concen a ion le els han he es o he samples. The
le els a e, in gene al, abo e 400 mBq g-1 o all adionuclides om he 238U
decay chain. These samples a e loca ed in he eas pa o he Sal és island
and he sou h o he No he n ma sh in he Odiel i e , all o hem along he
Odiel i e ups eam and downs eam om he e ilize indus ies. The
di e ence ound in he samples collec ed a he eas side o he Sal és island
mus , again, be ela ed o he composi ion o he samples. Thus, i can be
seen ha hose samples wi h low concen a ions (15 and 17) ha e densi y
and o ganic ma e alues e y di e en om he o he samples (16 and 18)
ha ha e qui e high concen a ions o adionuclides.
In gene al, excep ing he case o samples wi h di e en composi ion, he
di e ences in ac i i y concen a ion be ween samples seem o depend on
he loca ion o he sampling si es, which indica es he in luence o he
in low o Odiel i e wa e s o e each a ea. Thus, he bag o con aminan s
mo es ups eam and downs eam o he Odiel i e . Pa o i is clea ly
mo ing o he Odiel ma sh h ough he no h o he Bacu a island ha
la e lows in o he Moja e a channel.
We can also compa e ou esul s wi h o he da a ob ained in soils om
he a ea o Huel a, bu in he Tin o ma sh a ea (see Fig. 2) and a ound
he phosphogypsum piles (Boli a e al., 1995). Le els below 40 and
60mBqg-1 o 210Po and 238U, espec i ely, in s a ions loca ed in he eas
TABLE 1
Ac i i y Concen a ions (mBqg-1) o so ne Na u al Radionuclides om he U and Th Decay Chains in Soil Samples om he Odie! Ma sh
Collec ed in Feb ua y (F) and No embe (N) 1993
Code
O.M.(%)
21op0
238U 234u 232Th 230Th 22sTh
Fl
165 ± 7 189 ± 8
NI
10.8 199 ± 10 181 ± 8 197 ± 8 48.1 ± 2.5 186 ± 9 73.0 ± 7.0
N2
11.5 778 ± 41 698 ± 35 747 ± 37 88.1 ± 6.8 922 ± 52 160 ± 15
N3 14.8 643 ± 28 728 ± 32 751 ± 33 103 ± 5 898 ± 42 149 ± 13
N4 14.6 580 ± 26 540 ± 21 594 ± 23 61.1 ± 4.0 533 ± 26 144 ± 13
N13
15.4 222 ± 11 196± 7 217 ± 8 29.8 ± 1.8 112 ± 9 59.3 ± 6.3
F5 20.9 290 ± 31 360 ± 22 364 ± 22
N5 15.2 213 ± 10 232±9 248 ± 10 41.2 ± 3.0 208 ± 11 48.0 ± 3.3
N6 11.4 141 ± 7 147 ± 6 161 ± 6 31.0 ± 1.8 104 ± 5 14.0 ± 3.7
N7 13.1 130± 7 158 ± 6 179 ± 7 30.3 ± 2.2 125 ± 7 36.2 ± 2.5
N8
9.2 64.6 ± 4.0 64.8 ± 3.2 71.9 ± 3.5 26.6 ± 1.9 41.0 ± 2.6 30.9 ± 2.6
N9
9.7
188 ± 10 127 ± 5 142± 5 24.4 ± 1.6 101 ± 5 35.0 ± 4.0
FIO 12.9 25.1 ± 1.7 95.1 ± 4.9 116±6
NlO 12.7 27.9 ± 2.0 106±4 122± 5 23.6 ± 1.6 28.4 ± 1.9 22.5 ± 1.6
N23
14.5 210 ± 11 245±8 281 ± 9 41.4 ± 3.1 216 ± 13 62.1±5.4
N20 9.8 233 ± 11 258 ± 9
Nl8 17.3 565 ± 23 601 ± 21
Fl7 9.4 108±6 142 ± 10
N17 4.8 41.0 ± 3.2 17.6 ± 0.8
Fl6 13.7 367 ± 34 434 ± 16
Nl6 15.5 441 ± 20 511 ± 18
Nl5 4.6 131 ± 7 94.1 ± 3.7
Fl2 15.6 163 ± 9 147± 6
Nl2 9.3 44.2 ± 2.5 44.8 ± 1.6
Fll 13.3 124 ± 8 124 ± 6
Nll 9.2 194±9 75.4 ± 2.6
Nl9
5.7
54.4 ± 3.7 30.1±1.2
Fl4 12.5 40.5 ± 2.3 36.9 ± 1.6
N14 9.4 54.7 ± 3.9 37.8 ± 1.6
N21 1.1 16.2 ± 2.5 17.9 ± 0.8
N22 2.3 37.2 ± 2.5 32.4 ± 1.3
283 ± 10 44.l ± 3.6
630 ± 21 56.4 ± 3.8
163 ± 12
18.8 ± 1.0 26.5 ± 2.5
498 ± 23
523 ± 19 68.l ± 4.5
101 ±4 17.1±1.2
158±6
48.4 ± 1.8 26.7 ± 1.6
138 ±7
87.4 ± 3.0 22.0 ± 1.4
34.7 ± 1.4 15.4 ± 1.0
43.4 ± 1.8
43.7 ± 1.8 22.4 ± 1.6
19.3 ±0.9 4.9 ± 0.3
36.7 ± 1.4 11.8±0.7
256 ± 16
443 ± 22
30.0 ± 2.7
554 ± 23
87.4 ± 4.7
28.l ± 1.7
71.0 ± 3.7
31.7 ± 1.9
42.8 ± 2.7
8.8 ± 0.5
16.0 ± 0.9
78.5 ± 6.4
120 ± 12
32.8 ± 2.9
100 ± 12
46.3 ±4.5
25.0 ± 1.7
28.9 ±4.l
16.4 ± 1.3
22.5 ± 0.4
4.3 ± 0.9
13.3 ± 1.1
232Th/23su = 2_57e3su)-o.4ss
and
232Tb/230Tb = 3.14(23ºTh)-o.sos,
wi h eg ession coe icien s o -0.8623 and -0.9267, espec i ely.
(6)
(7)
These ela ionships may e lec ha hese ac i i y a ios emain
cons an only o concen a ions o 238U and 230Tb abo e so ne
200 mBq g-1• F o concen a ions below his alue, con amina ion o
adionuclides om he 232Tb decay chain seems o be undis inguished.
Spa ina densi lo a
The same adionuclides we e analysed in samples o Spa ina densi lo a,
whose esul s a e p esen ed in Table 2. The ac i i ies ange, in gene al,
om 2 o 50 mBq g-1 o 210Po and U iso opes, wi h he ac i i y concen
a ions o 21ºPo being highe han hose o U-iso opes in mos samples.
The e is a di e ence o one o de o magni ude be ween he highes and
he lowes concen a ions. As in he case o soil subs a es, he highes
concen a ions in Spa ina densi lo a we e ound a he No he n ma sh
and a he eas side o he Sal és island. Thus, in gene al, he highes
adioac i e concen a ions in plan s a e ound in hose collec ed in a eas
wi h he highes adioac i e concen a ion in he soil subs a e, and he
lowes in hose wi h he lowes concen a ions in he subs a e. Concen
a ions o 230Tb a e gene ally lowe han hose o 210Po and U-iso opes.
Howe e , he same pa e n o dis ibu ion is obse ed. Concen a ions o
adionuclides om he 232Tb decay chain a e clea ly much lowe han
hose o adionuclides om he 238U decay chain ( anging om 0.26 o
4.14 o bo h Th iso opes). In gene al, he concen a ion o 228Tb is highe
han ha o 232Tb. This ac should be ela ed wi h he highe mobili y o
228Ra. Howe e , i is also ue ha he adioac i e concen a ion o bo h
iso opes in plan s collec ed in he No he n ma sh and in he eas side o
he Sal és island a e highe han in hose samples collec ed in o he
s a ions.
I seems in e es ing o s udy he ela ionship be ween hese adio
nuclides. In Fig. 5(a), adioac i e concen a ions o bo h U iso opes a e
plo ed. I can be clea ly obse ed ha bo h iso opes a e qui e well linea ly
ela ed ( = 0.996), as was ound in he case o he soil subs a e samples.
Mo eo e , again he slope o he line (1.073 ± 0.018), o a y-axis in e cep
ze o (0.174 ± 0.262), would gi e he 234U /238U ac i i y a io o he plan .
Thus, he e is again a sligh excess o he daugh e iso ope. The ela ion-

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,s
"'u (mBqlg)
)•,.o
'·'
-2.CJ
�
.-,H
.,...,.,.,, ...
. ::
o
J.0
..
•
...... --.
_,... .
_,, • .§.. , 5
¡::.
0,5 ........ •
. . .
o
N ,.oj, . '; .
, .
1
o.o 1� 1!)
L-:_-, __ ;;;----;i;----io---215
""Th (mBQlgl
'º 25
10
1S
,,.U (mBqlg)
"
Fig. 5. Rela ionship be ween concen a ions o adionuclides om he
238U
decay chain in Spa ina densi lu a samples (a) 234U s.
238U,
(b)210po YS. 238U, (e) 230Tb s. 238u, (d) 228Th s. 232Th, (e) 232Th s. 238u and ( ) 232Th s. 230Th.
ship be ween he concen a ions o 210Po and ha o 238U [see Fig. 5(b)], is
no clea . Howe e , he e is s ill a clea end o inc easing 210Po concen
a ions when concen a ions o 238U inc ease ( = 0.8515). Compa ing
he U concen a ion in he plan wi h he y-in e cep o his line
(5.59 ± 1.45), he la e mus be conside ed clea ly di e en o ze o. This
y-in e cep e lec s he a ia ion in he 210Po/238U ac i í y a io wi h he
238U concen a íon in he plan . Thus, o a low U concen a íon (back
g ound le els), he e is an excess o 210Po compa ed o 238U. This excess
dec eases o secula equílíb íum o high 238U concen a íons. In ac , o
plan s wi h enhanced concen a ions, bo h adionuclídes a e p ac ically in
secula equilib ium.
Agaín, a linea ela ionship ( = 0.8223) can be ound be ween he 23ºTh
and 238U concen a ion in he plan s [see Fig. 5(c)]. In his case, he alue
close o ze o o he y-in e cep (0.368 ± 1.39) gi es a 23ºTh/238U ac i i y
a io qui e cons an ac oss all he a ea (0.638 ± 0.110). This alue o he
ac i i y a io e lec s a clea de ici y o 230Th in he plan s, opposi e o ha
ound in soils. This di e ence be ween ac i i y a ios in soils and plan s
can be explained by he lowe mobili y o Th compa ed o U.
Bo h Th iso opes om he same decay chain (232Th and 228Th) a e also
linea ly ela ed ( = 0.8950), as can be obse ed in Fig. 5(d). The alue o
he y-in e cep , gi es p ac ically secula equilib ium be ween iso opes in
all samples.
Mo e ín e es ing seems o be he ela ionship o he 232Th concen a
ions wi h he 238U and 230Th concen a ions [see Fig. 5(e) and 5( )]. The
concen a ion o 232Th in he plan clea ly inc eases as he concen a ion
o U and/o 23ºTh inc eases, ollowing linea ela ionships ( eg ession
coe icien s o O. 7220 and 0.9248, espec i ely). As hey a e iso opes o he
same elemen , he ela ionship be ween bo h Th iso opes is much be e .
In bo h cases, he y-axis in e cep is nea ly ze o, gi en 232Th/238U and
232Th/23ºTh ac i i y a ios o 0.087 ± 0.021 and 0.143 ± 0.015, espec
i ely.
Concen a ion a ios
We we e also ín e es ed in he s udy o he biological up ake and ans
e o hese adionuclides om he soil subs a e o he plan . Thus, we
ha e calcula ed he expe imen al alues o he concen a ion a ios o
each adionuclide in each s a ion. The esul s a e p esen ed in Table 3.
Fo 210Po, concen a ion a ios anging om 0.026 ± 0.002 o
0.948 ± 0.082, wi h a mean alue o 0.172 ± 0.204, we e ound. The
s anda d de ia ion o his mean alue e lec s he high dispe sion o he
da a. In ac , di e ences abo e one o de o magni ude a e ound.
Mo eo e , i is in e es ing o no ice ha di e en alues o his ac o
depend on he ac i i y concen a ion o he soil subs a e. Thus, high
concen a ion a ios appea in s a ions wi h low ac i i y concen a ions
in he subs a e, and low in mo e con amina ed s a ions. The same
occu s in he case o all adionuclides om he 238U decay chain. Fo
bo h U iso opes (238U and 234U), he expe imen al concen a ion a ios
ange om 0.022 ± 0.002 o 0.269 ± 0.03 l o 238U and om
0.024 ± 0.002 o 0.272 ± 0.032 o 234U, wi h mean alues o
0.083 ± 0.061 and 0.082 ± 0.060, espec i ely. Again, in bo h cases, he
concen a ion a io (CR) depends on he ac i i y concen a ion o he
elemen s in he soil subs a e. The same is ound in he case o he
concen a ion a io o 23ºTh. I anges om 0.010 ± 0.001 o
0.202 ± 0.022, wi h a mean alue o 0.065 ± 0.057. Thus, i seems ha
he beha iou o he concen a ion a io, which means he up ake by
plan s o adionuclides om i s subs a e, depends on he ac i i y
concen a ion o he elemen in he soil subs a e.
In he case o bo h Th iso opes om he 232Th decay chain, he
concen a ion a io anges om 0.014 ± 0.004 o 0.065 ± 0.008 o 232Th
and om 0.011 ± 0.001 o 0.084 ± 0.022 o 228Tb, wi h mean alues
0.036 ± 0.018 and 0.042 ± 0.025, espec i ely. The dispe sion o he da a
seems o be no as high as ha o adionuclides om he 238U decay
chain. Howe e , we mus conside ha , in his case, he ange o Th
concen a ion in he soil subs a e is no as wide as in he case o U and
daugh e s.
In o de o s udy he beha iou o he concen a ion a ios o hese
adionuclides, concen a ion a ios e sus he ac i i y concen a ion a he
adionuclide in he soil subs a e ha e been plo ed in Fig. 6 o 238U and
daugh e s and in Fig. 7 o 232Th and 228Tb. The CR alues clea ly
dec ease when he ac i i y concen a ion in he subs a e soil inc eases. In
ac , he da a can be modelled by i ing unc ions o he o m:
CR = aC� (8)
Thus, i b = O, his would mean ha he concen a ion a io is cons an ,
ega dless o he ac i i y concen a ion in he soil subs a e. Func ions o
his ype ha e been i ed o 210Po, 238U, 234U and 230Tb, and hese esul s
a e p esen ed in Table 4. Thus, o all adionuclides om he 238U, he b
alue o he hype bolic unc ion is clea ly di e en om ze o,
-0.750 ± 0.097, -0.445 ± 0.081, -0.438 ± 0.082 and -0.573 ± 0.098 o
210Po, 234U, 234U and 23ºTh, espec i ely. Howe e , he linea i y assump
ion may i be e in he case o U iso opes. Thus, i seems ha all hese
adionuclides ollow he beha iou o an essen ial elemen o he plan
TABLE4
Concen a ion Ra io (CR) Fi ed Func ions o Radionuclides om he 238U Decay Chain
Radionuclide
210p0
23su
234u
230Th
CR =aC
CR = 4.06 c;º·750
CR = 0.59 c;º·445
CR = 0.588 c,0·438
CR = 0.717 c,0573
l.96
0.239
0.247
0.349
0.097
0.081
0.082
0.098
-0.8296
-0.7137
-0.7030
-0.8256
C, means he concen a ion o he adionuclide in he soil subs a e.
g ow h. Mo eo e , i ac i i y concen a ions in he soil subs a e abo e
200mBqg-1 a e only conside ed, he CR alue would be appa en ly
cons an . Thus, conside ing only hose s a ions wi h high ac i i y concen
a ions in he soil subs a e, CR alues o 0.050 ± 0.023, 0.046 ± 0.020
and 0.023 ± 0.011 a e ob ained o 210Po, U-íso opes and 23ºTh, espec
i ely. In his case, i he CR alue is used o p edic plan concen a ions
om subs a e concen a ion, i will unde p edic plan concen a ion
when he subs a e concen a ion is less han ,..._, 200 mBq g-1. Sheppa d and
Sheppa d (1985) ound ha he CR o na u al U in na i e plan s a he
" 'T
. :T •
º·'
,
.. :
I
"
� º·'i
o.,�,-
.,_ ..
�--.-------� --. ------�---+- --·--+--
0.30
0.25
0,20
0::: 0,15
u
0,10
0.05
0.00
200
T
1
T
I
1!
· .} I
_{_
.! I
·. I
Pi. ·I.
...
200
<-00 800 800
C8 (mBq/g)
234u
I
j _
,oo 600
C. (mBqlgJ
800
O.JO :T
, 1 b
º·" .T
0.20
+-,-! ..
0:::: 0,15 J".1
ü ' �
0.25 '.
º·'° ·
,!
0.15 T
5 '
º·" l.
200
o.o, 'i:_ . I
..
I1í ··--]I;
J[
0.00 ¡
O 200
I
J: I
-- --- --- ---_]l_ -
,oo 600 800
C.(mBq/g)
·�-- -- -· -- -- ---------•.---
'
'°º '
600
C.(mBq/g)
' --,
800 1000
Fig. 6. Concen a ion a ios s. he ac i i y concen a ion o he elemen in he soil
subs a e o
(a) 210Po, (b) 238U, (e) 234U and (d) 23ºTh.
P ecamb ian Shield appea ed o be dependen upon subs a e concen a
ion below ""20 µgg-1. They assumed he use o he CR concep o p edic
U concen a ion in plan s o be alid when subs a e concen a íons a e
highe han abou 20 µgg-1• In ou case, his ac seems o be ue o ali
adionuclides om he 238U decay chain. The case o bo h Th iso opes
om he 232Th decay chain is no e y clea . The CR alues (see Fig. 7)
seem o be mo e o less cons an compa ed wi h hose o adionuclides
om he 238U decay chain, wi h mean alues o 0.036 ± 0.017 and
0,16 232Th
•
0,14
0,12
0,10
a::: 0.08
III
0,06 T I I
0,04 1
]: I l:
0,02 ]:
:q I I
º·ºº'
o20
40
60 80 100 120
C. (mBq/g)
b
0,10
• 1
!
+ I
1
0,05 -'--
I
II lI ! I
I
I I
0,00 +-���--.-�-.---..-----,--���--.�-.---..---.-�-,
o 20 40 60 80 100 1W 1� 100 100
C.(mBq/g)
Fig. 7. Concen a ion a ios s. he ac i i y concen a ion o he elemen in he soil
subs a e o (a) 232Th and (b) 228Th.

0.042 ± 0.025 o 232Th and 228Th, espec i ely . Howe e , he ange o
ac i i y concen a ion o hese adionuclides in he soil subs a e, should
be conside ed ca e ully.
Thus, i seems ha , when s udying he up ake o adionuclides by plan s
om i s subs a e concen a ion, i is necessa y o conside a easonably
wide ange o ac i i y concen a ion in he soil subs a e. O he wise,
no hing can be clea ly p edic ed. l seems ha a leas hose adionuclides
om he 238U decay chain beha e as essen ial elemen s o he g ow h o
he plan . Howe e , whe he hese elemen s a e essen ial o a e mimicking
essen ial elemen s canno be de e mined wi hin his s udy.
CONCLUSIONS
Concen a ions o 210 Po, U- and Th-iso opes in Spa ina densi lo a and
soil subs a e samples collec ed om a saline we ma sh ha e been s udied.
The ac i i y concen a ions show clea ly he in luence ha he adio
ac i i y con ained in he phospha e ock used o he phospho ic acid
p oduc ion has o e he concen a ion o na u al adionuclides in ce ain
zones o he ma sh, a ec ing he plan s and he soils. Indeed, he s a ions
mo e in luenced by he Odiel wa e s p esen he highes concen a ions in
soils and plan s.
Concen a ion a ios o all adionuclides in he plan we e de e mined.
The concen a ion a io o an elemen seems o be dependen on he
ac i i y concen a ion o he same elemen in i s soil subs a e. Thus, high
CRs appea in plan s g owing in soils wi h a low concen a ion o adio
nuclides, whe eas low CRs appea in plan s g owing in soils wi h high
concen a ions. Mo eo e , he ela ionship be ween he CR and he
ac i i y concen a ion o he soil subs a e seems o be hype bolic, a leas
in he case o adionuclides om he 238U decay chain. As a consequence,
i he CR alue is used o p edic plan concen a ions om subs a e
concen a ion, i will unde p edic plan concen a ion when he subs a e
concen a ion is less han "'200mBq g-1. Howe e , in he case o 232Tb
and 228Tb, he na ow ange o ac i i y concen a ion o hese adio
nuclides in he soil subs a e, could be he eason o he appa en
cons ancy o he CR wi h subs a e concen a ion.
ACKNOWLEDGEMENT
This wo k was pa ially suppo ed unde EC con ac FI 3P-CT920035.
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