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Determination of uranium and polonium in Sparus aurata by alpha spectrometry

Abstract

The aim of this study was optimizing conditions for the specific activities determination of some uranium-series radionuclides present in Sparus aurata by alpha spectrometry. Determinations of specific activities were conducted varying the type of digestion: acid attack on hot plate, controlled microwave digestion and acid attack after calcination of the sample. The latter procedure was applied only to the case of uranium isotopes determination. The variation in the isotope extraction method consisted of applying the techniques of liquid-liquid extraction using Tributyl phosphate (TBP) or chromatographic UTEVA resin. Results depending on the type of treatment given to the samples were compared based on obtained chemical yields. The results reveal a higher bioaccumulation of polonium in the liver sample, with activities of 0.809, 2.495 and 2.439 Bq kg-1 fresh wt compared with the fillet. The best chemical yields for polonium were close to 60% for samples that were digested by microwave. In the case of uranium the best chemical yields, close to 80% for fillet, were obtained with a previous calcination of the sample and using the UTEVA resin.

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Determination of uranium and polonium in Sparus aurata by alpha spectrometry

Author: Luna Porres, Mayra; Manjón Collado, Guillermo; Díaz, I.; Rentería Villalobos, Marusia; Montero Cabrera, María Elena
Publisher: Sociedad Mexicana de Física
Year: 2012
Source: https://idus.us.es/bitstreams/04f9bfe0-ab81-4934-8fbb-287435b3fd8d/download
Re is a Mexicana de Física
ISSN: 0035-001X
[email p o ec ed]
Sociedad Mexicana de Física A.C.
México
Luna Po es, M.; Manjón Collado, G.; Díaz, I.; Ren e ía, M.; Mon e o Cab e a, M.E.
De e mina ion o u anium and polonium in Spa us au a a by alpha spec ome y
Re is a Mexicana de Física, ol. 58, núm. 3, junio, 2012, pp. 224-227
Sociedad Mexicana de Física A.C.
Dis i o Fede al, México
A ailable in: h p://www. edalyc.o g/a iculo.oa?id=57023406009
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RADIATION PHYSICS Re is a Mexicana de F´
ısica 58 (2012) 224–227 JUNIO 2012
De e mina ion o u anium and polonium in Spa us au a a by alpha spec ome y
M. Luna Po es1, G. Manj´
on Collado2, I. D´
ıaz2, M. Ren e ´
ıa1, M.E. Mon e o Cab e a1∗
1Cen o de In es igaci´
on en Ma e iales A anzados, S.C.,
Miguel de Ce an es 120, Complejo Ind. Chihuahua, Chihuahua, Chih., M´
exico
2Depa amen o de F´
ısica Aplicada II de la Escuela T´
ecnica Supe io de A qui ec u a,
Uni e sidad de Se illa, Espa˜
na.
∗Co esponding au ho : elena.mon e o@cima .edu.mx
Recibido el 3 de junio de 2011; acep ado el 4 de eb e o de 2012
The aim o his s udy was op imizing condi ions o he speci ic ac i i ies de e mina ion o some u anium-se ies adionuclides p esen in
Spa us au a a by alpha spec ome y. De e mina ions o speci ic ac i i ies we e conduc ed a ying he ype o diges ion: acid a ack on
ho pla e, con olled mic owa e diges ion and acid a ack a e calcina ion o he sample. The la e p ocedu e was applied only o he case
o u anium iso opes de e mina ion. The a ia ion in he iso ope ex ac ion me hod consis ed o applying he echniques o liquid-liquid
ex ac ion using T ibu yl phospha e (TBP) o ch oma og aphic UTEVA esin. Resul s depending on he ype o ea men gi en o he
samples we e compa ed based on ob ained chemical yields. The esul s e eal a highe bioaccumula ion o polonium in he li e sample,
wi h ac i i ies o 0.809, 2.495 and 2.439 Bq kg−1 esh w compa ed wi h he ille . The bes chemical yields o polonium we e close o
60% o samples ha we e diges ed by mic owa e. In he case o u anium he bes chemical yields, close o 80% o ille , we e ob ained
wi h a p e ious calcina ion o he sample and using he UTEVA esin.
Keywo ds: U anium; polonium; alpha spec ome y; ish.
El obje i o de es e es udio ue la op imizaci´
on de las condiciones pa a la de e minaci´
on de las ac i idades espec´
ı icas de algunos adion´
uclidos
de la se ie del u anio p esen e en Spa us au a a po espec ome ´
ıa al a.Las de e minaciones de las ac i idades espec´
ı icas se ealiza on
a iando el ipo de diges i´
on: a aque ´
acido en pa illa, en mic oondas y a aque ´
acido despu´
es de la calcinaci´
on de la mues a. Es e ´
ul imo
p ocedimien o ue aplicado solamen e en el caso de la de e minaci´
on de los is´
o opos de u anio. La a iaci´
on en el m´
e odo de ex acci´
on
del is´
o opo, consis i´
o en la aplicaci´
on de las ´
ecnicas de ex acci´
on l´
ıquido-l´
ıquido u ilizando el os a o de ibu ilo (TBP) o sepa aci´
on
c oma og ´
a ica empleando la esina UTEVA. Los esul ados ob enidos en los di e en es ipos de a amien os que se les dio a las mues as,
ue on compa ados con los endimien os qu´
ımicos ob enidos. Los esul ados e elan una mayo bioacumulaci´
on de polonio en la mues a
de h´
ıgado, con ac i idades de 0.809, 2.495 y 2.439 Bq kg−1de peso esco en compa aci´
on con el ile e.Los mejo es endimien os qu´
ımicos
pa a el polonio ue on ce canos al 60% pa a las mues as que se some ie on a diges i´
on po mic oondas. En el caso del u anio los mejo es
endimien os qu´
ımicos, ce canos al 80% en ile e, se ob u ie on con una calcinaci´
on p e ia de la mues a y el uso de la esina UTEVA.
Desc ip o es: U anio; polonio; espec ´
ome o al a; peces.
PACS: 91.62.+g; 89.60.-k.
1. In oduc ion
The impo ance o s udying con amina ion le els by hea y
me als and me alloids (HMM) in he aqua ic en i onmen is
due o he ac ha HMM a ebioaccumula i e, no biodeg ad-
able, and may be easily inco po a ed in o he ood chain.
This con amina ion may ha e se ious e ec s on human
heal h [1,2].
O ganisms wi h me als in hei issues a e o en used
o indica e and quan i y he le els o con aminan s o hei
bioa ailabili y in he en i onmen . A bioindica o is an o -
ganism ha con ains in o ma ion abou he quali y o he
en i onmen ; a biomoni o con ains in o ma ion abou he
quan i a i e aspec s o he quali y o he en i onmen [3,4].
In he ma ine en i onmen di e en o ganisms such as oys-
e s, sh imp and ish [5] ha e been used o con amina ion
moni o ing.
Fish a e ideal indica o s o pollu ion because hey occupy
di e en ophic le els; u he mo e, ish samples a e o di -
e en sizes and ages [1].
The up ake o adionuclides by ish depends on a iables
such as die a y habi s, loca ion, ish physiology and physical-
chemical a iables such as pH, empe a u e and wa e (in-
cluding he concen a ion o adionuclides) [6].
The Po-210 en e s he human body ia inhala ion o
adon gas Rn-222 and inges ion o ood and wa e , inges-
ion o ood being he majo ou e [7]. Ma ine bio a ha e
been ound o con ain high concen a ions o Po-210, which
is conside ed o be he majo con ibu o o adia ion dose e-
cei ed by man (abou 0.11 mS yea −1)[8, 9]. The e o e,
many coun ies and se e al in e na ional o ganiza ions ha e
de e mined he concen a ions o his adionuclide in sea ood
[7].The objec i e o his s udy was op imizing he p ocedu e
o he de e mina ion o speci ic ac i i ies o some u anium-
se ies adionuclides p esen in Spa us au a a by alpha spec-
ome y.
This species was selec ed o he p esen s udy because i
is a med in almos all Medi e anean coun ies and i s size
can a y om 20 o 57 cm. These a e impo an ac o s o
DETERMINATION OF URANIUM AND POLONIUM IN SPARUS AURATA BY ALPHA SPECTROMETRY 225
conside ing i as a possible biomoni o o con amina ion by
adionuclides.
2. Ma e ials and me hods
Fish samples we e ob ained om a local supe ma ke a he
ci y o Se ille in Spain .The a ge species was Spa us au a a
(commonly known as ”Golden”). Se en ish samples we e
used o he adiochemical analysis. Fish sizes a ied om
26 o 28 cm o leng h, o no in oducing size o age as a
a iable in ou analysis.
2.1. Sample p epa a ion
Be o e dissec ion, he samples we e washed ho oughly wi h
dis illed wa e and hen hey we e measu ed and weighed.
Subsequen ly he ish we e sepa a ed o analysis in o h ee
pa s: li e , edible ille and bone; he weigh s o hese
h ee pa s we e eco ded o u he calcula ions. Biological
samples we e lyophilized o i e days o ex ac he wa e .
Weigh s we e eco ded o ge he mois u e loss and inally,
se en samples o each pa o he ish we e combined and
homogenized be o e he analysis.
2.2. Radiochemical me hods and measu emen ech-
niques
Samples we e subjec ed o adiochemical analysis o Po-210,
U-234 and U-238. The p ocedu es employed we e p e iously
desc ibed [10, 11]. The s anda ds yield ace s used ( om
Iso ope P oduc s) we e Po-209 (Ac i i y=172.7±5.2 mBq/g)
and U-232 (Ac i i y=117.8±0.6 mBq/g).
Alpha spec ome y wi h su ace ba ie silicon PIPS de-
ec o s ( om CANBERRA) was he me hod applied o de e -
mine he speci ic ac i i ies in ish samples.
Gene al p ocedu e o he diges ion o samples is p e-
sen ed in Figu e 1.
2.2.1. Polonium de e mina ion
A s anda d yield ace Po-209 was added in di e en quan i-
ies o ish samples which we e diges ed by mic owa e o ho
pla e.
Au odeposi ion o polonium was done by using asco bic
acid in HCl solu ion, hen solu ion was hea ed o 80oC and
Powas spon aneously pla ed on o a o a ing coppe disc. Po-
210 ac i i y was co ec ed o eco e y by compa ison wi h
he measu ed ac i i y o he Po-209 yield ace .
FIGURE 1. Gene al p ocedu e o sample diges ion.
2.2.2. U anium de e mina ion
A s anda d yield ace U-232 was added in di e en quan i-
ies o ish samples which we e diges ed by calcina ion o in
solu ion wi h a ho pla e.
The iso ope ex ac ion me hods applied we e liquid-
liquid ex ac ion wi h ibu yl phospha e (TBP) and ch o-
ma og aphic UTEVA esin. The iso ope ex ac ion me hods
a e based on he me hod ini ially de eloped [12-14].
The men ioned ex ac ion me hods a e p esen ed in Fig-
u es 2 and 3.
Figu e 3 shows he low diag am o u anium and ho ium
ch oma og aphic sepa a ion wi h UTEVA esin. The diges ed
sample is pou ed on he esin and hen 5 mL HNO33M is
added. The ex ac ion me hod o ho ium and u anium is
pe o med sequen ially by adding acids solu ion in concen-
a ions shown by he a ows in s ep 3 and 4.
U anium was elec odeposi ed om he solu ion on a pol-
ished s ainless-s eel disc, using Halls adius me hods [15].
The cell used o his elec odeposi ion is made o e lon
which p e en s he adionuclides om adso bing on he wall
o he cell [10, 15-17].
FIGURE 2. Liquid - liquid ex ac ion echnique.
FIGURE 3. Ch oma og aphic sepa a ion echnique using UTEVA
esin.
Re . Mex. Fis. 58 (2012) 224–227
226 M. LUNA PORRES, G. MANJ´
ON COLLADO, I. D´
IAZ, M. RENTER´
IA, M.E. MONTERO CABRERA
TABLE I. Po-210 ac i i y concen a ions gi en on esh weigh ba-
sis, ob ained o di e en ypes o sample ea men and di e en
sample issues. F means ille and L means li e .
SAMPLES Po-210 YIELDS TREATMENTS
(Bq kg−1) (%)
S1-F 0.21±0.03 27 Ho pla e
S2-F 0.16±0.03 28 Ho pla e
S3-F 0.44±0.08 11 Ho pla e
S4-F 0.15±0.02 61 Mic owa e
S5-F 0.12±0.02 62 Mic owa e
S6-F 0.14±0.02 56 Mic owa e
S1-L 2.50±0.13 66 Mic owa e
S2-L 2.44±0.13 60 Mic owa e
S3-L 0.81±0.11 61 Mic owa e
3. Resul s and discussion
The da a ob ained om he adiochemical analysis o
Po-210, U-234 and U-238 in all ish samples a e p esen ed
on he basis o esh weigh .
3.1. Polonium concen a ion in ish edible ille and li e
Figu e 4 p esen s an alpha spec um o polonium iso opes ex-
ac ed o a ish sample, showing bo h Po-210 and ace Po-
209 lines. The da a ob ained om he adiochemical analysis
o Po-210 in ish samples a e p esen ed in Table I. I shows
ha he chemical yields a ained o samples diges ed in ho
pla e a e e y low, a ying be ween 11.25% and 28.04%. I
was obse ed a yellowish suspension, sugges ing ha his
p ocedu e does no ully diges he lipids p esen in he sam-
ples, and hen i hinde he p ecipi a ion p ocess o ac inide
necessa y a e diges ion. By con as , mic owa e sample di-
ges ion p oduced chemical yields abou 60%, because diges-
ion o lipids p esen in he ish sample was almos comple e.
De e mina ion o polonium concen a ion in sea ish
muscle in Sy ia shows concen a ions abou 0.12±0.01 and
0.13±0.042 Bq kg−1we weigh s o he species Spa us au-
a a [7]. Resul s ob ained in he p esen wo k o he same
species (see Table I a e o he same o de o magni ude as
hose epo ed in [7], pa icula ly o hose ob ained by mi-
c owa e diges ion p ocedu e. The di e ences be ween al-
ues epo ed in he p esen wo k and hose epo ed in [7]
may be jus i ied acco ding o eeding pa e ns and concen a-
ions o polonium p esen in he aqua ic en i onmen whe e
ish li e.
Polonium in li e samples showed he highes speci ic ac-
i i y alues (see Table I). This is expec ed because his o gan
ypically bioaccumula es mo e polonium [18].
FIGURE 4. Alpha spec um o polonium iso opes, in loga i hmic
scale, ex ac ed om a ish li e sample.
TABLE II. U-238 and U-234 ac i i ies concen a ions, gi en on esh weigh basis, ob ained o di e en ypes o sample ea men .
No e: LD deno es below de ec ion limi = 0.004 Bq/kg.
SAMPLES U-234 U-238 YIELDS U-234/U238 TREATMENTS
(Bq kg−1) (Bq kg−1) (%)
S1-F LD LD 38.15 - Ho pla e UTEVA esin
S2-F LD LD 25.41 - Ho pla e TPB
S3-F LD LD 10.05 - Ho pla e TPB
S4-F 0.008±0.002 0.005±0.001 83.96 1.67 Calcina ion UTEVA esin
S5-F 0.007±0.001 0.005±0.001 68.62 1.33 Calcina ion TPB
S6-F 0.012±0.001 0.008±0.0005 59.73 1.37 Calcina ion TPB
S7-F LD LD 79.50 - Calcina ion UTEVA esin
S1-B 0.28±0.05 0.74±0.17 10.89 0.38 Calcina ion UTEVA esin
S2-B 0.27±0.03 0.57±0.18 3.73 0.47 Calcina ion TPB
Re . Mex. Fis. 58 (2012) 224–227
DETERMINATION OF URANIUM AND POLONIUM IN SPARUS AURATA BY ALPHA SPECTROMETRY 227
3.2. U anium concen a ion in ish edible ille and
bone.
The da a ob ained om he adiochemical analysis o U-234
and U-238 in ish samples a e p esen ed in Table II. I shows
ha he chemical yields achie ed o samples diges ed by
acid a ack on he ho pla e a e e y low, a ying be ween
10% and 38%. By con as , he calcina ion o he samples be-
o e acid a ack o diges ion p oduced chemical yields abou
60%, because i ensu es he diges ion o ma e ial ha could
in e e e wi h u anium de e mina ion (see Table II).
In he case o bone samples, i was no possible o
achie e good measu emen s because calcium ( e y abun-
dan in bones) in e e ed wi h he p ecipi a ion o ac inides.
The e o e, de eloping p ocedu es o a oid in e e ence by
calcium is needed o u anium de e mina ion in bone.
4. Conclusions
The bes al e na i e o de e mining u aniumin ille and li e
biopsies is he calcina ion o he samples be o e acid a ack
o diges ion, ollowed by UTEVA esin ex ac ion. This is
a as e p ocedu e, highe chemical yields a e ob ained and i
ensu es u anium measu emen in he sample. The bes p oce-
du e o polonium de e mina ion was ob ained by mic owa e
diges ion. De eloping p ocedu es o a oid in e e ence by
calcium o u anium de e mina ion in bone is sugges ed.
Acknowledgemen s
This esea ch has been pa ially suppo ed by Becas Mix as
CONACYT and he Uni e si y o Se ille, Spain. Au ho s
wan o hank C. Solis o sugges ions and ui ul discus-
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