POLONIUM-210 AND LEAD-210 IN THE BRAZILIAN SARDINE Sardinella brasiliensis

AND THE CHEMICAL COMPOSITION OF ORGANS AND TISSUES

Alphonse Kelecom1, Wagner de Souza Pereira2,3, Eliane Teixeira Mársico4, Sérgio C. São Clemente4 and Rita de

Cássia S. Gouvea1

3rd International Conference on Po and Radioactive Pb Isotopes11-14 October 2015 - Kusadası / TURKEY

1. Laboratory of Radiobiology and Radiometry - UFF 2. Laboratory of Wastewater Monitoring - UVA

3. Coordinating Group for Radiological Protection - INB4. Department of Foodstuffs Technology - UFF

1st International Conference on Po and Radioactive Pb isotopesOctober 2009 - Sevilla/ España

List 1: Top 20 Articles, in the Domain of Article 21296469, Since 2011 (publication date of the domain article)

1. Increase of 210Po levels in human semen fluid after mussel ingestion.

Kelecom A, Gouvea R de C.J Environ Radioact; 2011 May;102(5):443-7.

2. Time-related increase in urinary testosterone levels and stable semen analysis parameters after bariatric surgery in men.Legro RS, Kunselman AR, Meadows JW, Kesner JS, Krieg EF, Rogers AM, Cooney RN.Reprod Biomed Online; 2015 Feb;30(2):150-6.

3. 'Mussel Ingestion': Top Publications.

BioMedLib Review OC; ;MusselIngestion:708300192. ISSN: 2331-5717. 2015/6/23; updates online.

4. Levels of 210Po and 210Pb in mussel and sediments in Candarlı Gulf and the related dose assessment to the coastal population.Aközcan S.Mar Pollut Bull; 2013 Aug 15;73(1):11-5.

5. IL-18 levels in the semen of male infertility: semen analysis.Qian L, Zhou Y, Du C, Wen J, Teng S, Teng Z.Int J Biol Macromol; 2014 Mar;64:190-2.

6. Pattern of semen fluid abnormalities in male partners of infertile couples in Riyadh, Saudi Arabia.AlEnezi H, Isa AM, Abu-Rafea B, Madbouly K, Binsaleh S.Can J Urol; 2014 Jun;21(3):7322-5.

7. Comparison of before and after varicocelectomy levels of nitric oxide in seminal fluid of infertile men.Keyhan H, Dadvar A, Ansari M, Rafiee K.Nephrourol Mon; 2012;4(4):629-32.

8. Seasonal and spatial variations of 210Po and 210Pb activity concentrations in Mytilus galloprovincialis from Croatian coast of the Adriatic Sea.Rožmarić M, Rogić M, Benedik L, Štrok M, Barišić D.Chemosphere; 2013 Nov;93(9):2063-8.

Thank you Prof. Tenório

Sardinella brasiliensis (Steindachner 1879)

2 cm

g w-6 /100 g fish

Sardinella brasiliensis• rich source of low cost

protein and of insaturated fatty acids (w-6 )

• one of the low cost fish most consumed in Brazil by poor populations

Material and Methods• 10 fresh specimens of S. brasiliensis were harvested from the

São Pedro fish market, city of Niterói, state of Rio de Janeiro, Brazil.

• Fish was caught off the city of Cabo Frio, RJ on the same day.

• Fishes were weighted (mean ± SD: 61.7±13.0 g; min-max: 47.0-77.2 g),

• measured (mean ± SD: 16.3±1.2 cm; min-max: 15.0-19.0 cm)

• and dissected to obtain samples of heart, eyes, gills, stomach, pyloric caeca, liver, gut, muscle and red muscle.

• All the remaining tissues (fins, skin, head, scales, …) were pooled and named residues.

tissue Distrib. of weight (%) *

Polonium-210 (CA) Distribution of 210Po

activities (%)CF

Normali-zation $

mean±SD min-max

gill 3.2 89.5±43,7 34.8-158.7 1.7 24,961 6

eye 1.0 133.7±67.3 57.7-277.8 0.8 32,326 8

heart 0.5 214.3±136.4 81.1-513.2 0.6 77,219 13

stomach 1.2 317.0±202.7 35.0-650-2 2.2 125,864 20

liver 0.8 850.6±682.5 120.3-2100.2 3.9 296,464 53

pyloric caeca (n=6) 8.2 1228.6±159.1 1045.4-1332.1 59.1 477,769 74

gut 2.4 1634.6±806.3 499.7-2596.0 22.8 709,230 102

muscle 65.5 16.0±4.5 9.6-24.0 6.1 4,848 1

red muscle 11.9 32.3±26.8 15.3-95.5 2.2 7,341 5

residues ** 5.4 15.0 - 0.5 - -

whole fish 100 64.6 *** 100 71,700 -

Table 1. Concentrations of activity (mBq g-1, mean ± SD) of 210Po in tissues and organs of Sardinella brasiliensis.

Unless otherwise stated, the number of replicates is 10. * % wet weight relative to the mass of the whole fish; ** fins, skin, head, bones and scales; *** calculated; $ ratio 210Po in a tissue/210Po in the muscle.

210Po 0.88

mBq L-1

within the latitudes of 0-15ºS

tissue Distrib. of weight (%) *

Lead-210 (CA) Distribution of 210Pb

activities (%)CF

Normali-zation

$mean±SD min-max

gill (n=9) 3.2 7.6±4.2 4.4-16.8 3.0 1,090 3

eye 1.0 8.3±3.9 3.7-16.1 1.0 1,037 4

heart 0.5 16.1±15.2 3.8-49.5 1.0 2,984 7

stomach 1.2 18.8±12.9 5.7-42.5 2.8 3,843 9

liver 0.8 29.9±30,1 2.1-92.6 2.9 5,366 14

pyloric caeca (n=2) 8.2 32.6±6.2 28.2-37.0 33.1 6,525 15

gut 2.4 67.0±23.0 33.2-106.3 19.7 14,947 31

muscle (n=9) 65.5 2.2±2.9 0.5-9.4 17.6 339 1

red muscle (n=9) 11.9 6.2±12.1 0.6-38.2 9.1 956 3

residues** 5.4 15.0 - 9.9 - -

whole fish 100 2.89 *** - 100 1,650 -

Table 2. Concentrations of activity (mBq g-1, mean ± SD) of 210Pbin tissues and organs of Sardinella brasiliensis.

Unless otherwise stated, the number of replicates is 10. * % wet weight relative to the mass of the whole fish; ** fins, skin, head, bones and scales; *** calculated; $ ratio 210Po in a tissue/210Po in the muscle.

210Pb 1.75

mBq L-1

within the latitudes of 0-15ºS

heart gill

eye

stomac

hliv

ergu

t

pyloric

caeca

muscle

red muscl

e0

200

400

600

800

1000

1200

1400

1600

1800

214.

3

89.5 133.

7 317.

0

850.

5

1634

.6

1228

.5

16.0

32.3

16.1

7.6

8.3 18.8

29.9

67.0

32.6

2.2

6.2

210Po (blue) and 210Pb (red) concentrations of activities (CA) in tissues and organs of S. brasiliensis.

heart gill eye stomach liver gut pyloric caecae

muscle red muscle

0

200

400

600

800

1000

1200

1400

1600

1800

214.3089.50 133.70

316.95

850.55

1634.59

1228.55

16.00 32.29

Distribution of 210Po in Sardinella brasiliensism

Bq/

g

heart gill eye stomach liver gut pyloric caecae

muscle red muscle

0

10

20

30

40

50

60

70

80

16.10

7.60 8.34

18.82

29.93

66.99

32.63

2.186.20

Distribution of 210Pb in Sardinella brasiliensis

mB

q/g

Conclusions

As expected from literature, 210Po and 210Pb concentrations of activities were:

• low in muscle,

• medium in heart, eyes and gills, and

• high in all the organs of the digestive tract

In addition the 210Po CA were c.a. 8-40 times higher than those of 210Pb.

residues0.5%

heart0.6%

gill1.7%

eye0.8%

stomach2.2%

liver3.9%

gut22.8%

pyloric caeca 59.1%.

muscle6.1%

red muscle 2.2%

Conclusions• Although muscle (including red muscle)

represent ~77% of the total fish weight, it contains only 8.3% of the total 210Po content, and 26.7% of the 210Pb one.

• On the contrary, the digestive tract organs that represent together only 13.8% of the fish weight contain up to 88.0% and 58.5% of the total 210Po and 210Pb activities respectively.

Distributions of 210Po and 210Pb CA in Sardinella brasiliensis

Po

heart0.5%

stomach1.2%

liver0.8%

gill3.2%

gut2.4%

muscle65.5%

red muscle11.9%

eye1.0%

pyloric caeca8.2%

residues5.4%

Distribuition of masses

residues9.9%

heart1.0%

gill3.0% eye

1.0%

stomach2.8%

liver2.9%

gut19.7%

pyloric caeca33.1%

muscle17.6%

red muscle9.1%

Pb

residues0.5%

heart0.6%

gill1.7%

eye0.8%

stomach2.2%

liver3.9%

gut22.8%

pyloric caeca 59.1%.

muscle6.1%

red muscle 2.2%

Distributions of 210Po and 210Pb CA in Sardinella brasiliensis

Po

heart0.5%

stomach1.2%

liver0.8%

gill3.2%

gut2.4%

muscle65.5%

red muscle11.9%

eye1.0%

pyloric caeca8.2%

residues5.4%

Distribuition of masses

residues9.9%

heart1.0%

gill3.0% eye

1.0%

stomach2.8%

liver2.9%

gut19.7%

pyloric caeca33.1%

muscle17.6%

red muscle9.1%

Pb

Residues:fins skin head

bones and scales

Conclusions

• Remarkably, fish residues contain proportionally 20 times more 210Pb (9.9%) than 210Po (0.5%). This reflects the higher affinity of lead for the fins, scales and principally bones.

• Considering the whole fish, the CF of 210Po (71,700) is 40 times that of

210Pb (1,650).

Fishwhole

fish muscle red muscle gill eye heart stomach liver pyloric

caeca gut

S. brasiliensis 71.7 4.8 7.3 24.9 32.3 77.2 125.9 296.5 477.8 709.2

C. micro-lepidatus

18.7 1.6 - 34.4 16.2 37.7 131.4 184.3 - 1845.4

G. brasiliensis 4.6 0.4 - 6.3 6.3 6.7 9.2 80.2 - 55.8

Table 3. CF for 210Po in tissues and organs of Sardinella brasiliensis compared to the CF values for Cynoscion microlepidatus and Genypterus brasiliensis

captured at the same niche (Mársico et al., 2014). (seawater = 0.9 mBq L-1) (Cherry and Heyraud, 1988), [All values must be multiplied by 1000].

Conclusions• Comparing the CF of 210Po reported here, it appears that the sardine accumulates much

more 210Po, except for the gut. This reflects both different feeding pattern, and the higher position in the food-chain of Clupeidae.

• Given that a single meal of sardine consists generally of four to six filets (~130-200 g), such a meal would supply 2080-3200 mBq of 210Po, and up to the double amount considering the more tasteful red muscle.

• Undoubtedly, by time, this may have a reflex on the internal dose of the consumer.

tissue 210Po/210Pb trend

gill 11.8 1.6eye 16.0 2.2heart 13.3 1.8stomach 16.8 2.3liver 28.4 3.9pyloric caeca 36.4 5.0gut 24.4 3.3muscle 7.3 1.0red muscle 13.2 1.8

Table 4. Ratios 210Po/210Pb in S. brasiliensis and trend to accumulate 210Po better than 210Pb as compared to this trend in muscle.

Conclusions

• The 210Po/210Pb ratios confirm the better accumulation of 210Po . • Clearly, 210Po in S. brasiliensis is not entirely supported by its grandfather 210Pb. • Thus, the marine environment seems to be a better source of 210Po than 210Pb, or fish are

more efficient in 210Po capture and/or in 210Po bioaccumulation.

tissue humidity lipids ashes proteins

gill 74.90 5.99 5.95 14.25

eye 78.24 6.28 1.32 18.91

heart 67.57 2.02 1.79 17.75

stomach 64.26 6.91 1.76 20.44

liver 54.82 20.74 1.91 20.36

pyloric caeca n.d. n.d. n.d. n.d.

gut 60.95 16.24 1.53 13.68

muscle 72.73 4.07 1.59 20.25

red muscle n.d. n.d. n.d. n.d.

Table 5. Chemical composition of S. brasiliensis.(n.d.: not dertermined)

Conclusion• Unexpectedly, the gut that contains most of the 210Po is poor in proteins, although

210Po is reported to bind preferentially to free SH groups, expected to be abundant in proteins.

Fig. 2. Correlations of the levels of

210Po and 210Pb with chemical

parameters.

h

Conclusions

• Although part of Po in S. brasiliensis is not supported by Pb, statistical analysis showed as expected high positive correlation of Po and Pb (Fig. 2).

• It also indicated good correlation of both Po and Pb with lipids, but unexpectedly no correlation with protein content.

Fig. 3 PCA multivariate analysis of the levels of 210Po and 210Pb with chemical parameters.

h

Conclusions

• Multivariate analyses (cluster and PCA) indicated a very similar behavior of Po and Pb and constitute a group that correlates to some extend with the lipid content in agreement with the univariate analysis (Fig. 3).

• On the other hand, water content and ashes also showed some similar behavior, but surprisingly protein content did not correlate satisfactorily with none of the other parameters.

ReferencesAarkrog, A., Baxter, M.S., Bettencourt, A.O., Bojanowski, R., Bologa, A., Charmasson, S., Cunha, I., Delfanti, R., Duran, E.,

Holm, E., Jeffree, J., Livingston, H.D., Mahpanya wong, S., Nies, H., Osvath, I., Pingyu, Li, Povinec, P.P., Sanchez, A., Smith, J.N., Swift, D., 1997. A comparison of doses from 137Cs and 210Po in marine food: a major international study. Journal Environ mental Radioactivity 34, 69-90.

Carvalho, F. P., Oliveira, J. M., Malta, M., 2011. Radionuclides in deep-sea fish and other organisms from the North Atlantic Ocean. ICES Journal of Marine Science, 68(2), 333–340.

Cherry, R.D. and Heyraud, M., 1988. Lead and Polonium in the world’s oceans. In Inventories of selected radionuclides in the oceans. IAEA-TECDOC-481, IAEA, Vienna, pp. 139-158.

Cherry, R.D. and Shannon, L.V., 1974. The alpharadioactivity ofmarine organisms. Atomic Energy Review 12,1-45.Heyraud, M., Cherry, R.D. and Dowdle, E.B., 1987. The subcellular localization of natural 210Po in the hepatopancreas of

the rock lobster (Jasus lalandii). Journal of Environmental Radioactivity 5 ,249-260.Hill, C.R., 1965. Polonium-210 in man. Nature 208: 423-428.Instituto Adolfo Lutz (São Paulo - Brasil), 2005. Métodos físico-químicos para análise de alimentos: normas analíticas do

Instituto Adolfo Lutz. 4ª ed. Brasília (DF): ANVISA. Kelecom, A., Gouvea, R.C.S., Santos, P.L., 2002. Levels of 210Po and 210Pb in cigars. Journal Radioanalytical and Nuclear

Chemistry 253, 129-133.Mársico, E.T. Ferreira, M.S., São Clemente, S.C., Gouvea, R.C.S., Jesus, E.F.O., Conti, C.C., Conte Jr, C.A. and Kelecom, A.

2014. Distribution of Po-210in two species of predatory marine fish from the Brazilian coast. J. of Env. Rad. 128:91-96.Parfenov, Yu.D., 1974. Polonium-210 in the environment and in the human organism. Atomic Energy Review 12, 75-143. Pentreath, R., 1977. Radionuclides in marine fish. Oceanography and Marine Biology Annual Review 15, 365-460.Pereira, W.S., Gouvea, R.C.S., Santos, P.L., Kelecom, A., 2001. Distribuição corpórea de 210Po e 210Pb no peixe Mugil

curema (Valenciennes, 1836) na Baía de Sepetiba, RJ-Brasil, in: Moraes, R., Crapez, M., Pfeiffer, W., Farina, M. , Bainy, A., Teixeira, V.L., Arte & Ciência (Eds.), Efeitos de Poluentes em Organismos Marinhos, São Paulo, pp. 183-195.

Smith-Briggs, J.L., Bradley, E.J., 1984. Measurements of natural radionuclides in U.K. diet. The Science of the Total Environment 35, 431-440.

Smith-Briggs, J.L., Bradley, E.J., Potter, M.D., 1986. The ratio of lead-210 to polonium-210 in U.K. diet. The Science of the Total Environment 54, 127-133.

Ugur, A., Yener,G. and Bassari, A., 2002. Trace metals 210Po (210Pb) concentrations in mussels (Mytilus galloprovincialis) consumed at western Anatolia. Applied Radiation and Isotopes 57, 565-571.

ObrigadoThank You