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1 IAEA-TECDOC-329 BEHAVIOUR OF RADIONUCLIDES RELEASED INTO COASTAL WATERS LITERATURE REVIEW

2 BEHAVIOUR OF RADIONUCLIDES RELEASED INTO COASTAL WATERS IAEA, VIENNA, 1985 IAEA-TECDOC-329 Printed by the IAEA in Austria February 1985

3 PLEASE

4

5 CONTENTS FOREWORD...

6 5. HABIT SURVEYS

7 3. LA REGION NORD-COTENTIN - LE CAP DE LA HAGUE Courantologie locale Morphologie et sédimentologie littorales

8

9 FOREWORD The Convention on the Prevention of Marine Pollution by Dumping of Wastes and Other Natter (London, 1972) conferred upon the IAEA the responsibility for defining levels and making recommendations to National Authorities

10 At the same time, in order to have available a preliminary basis for judgement, the Agency has entrusted two consultants' groups with the preparation

11 ~ The three case studies ; these were prepared within a commonly agreed framework

12 AVANT PROPOS La Convention sur la prévention de la pollution marine par immersion de déchets

13 Dans

14

15 In preparing this material EDITORIAL NOTE

16 HISTORY July Advisory Group Meeting on "Considerations concerning de minimis quantities

17 Results

18 GENERAL REVIEW OF LITERATURE RELEVANT TO COASTAL WATER DISCHARGES Compued

19 1. INTRODUCTION Artificially-produced radionuclides have been introduced into the marine environment since 1944, when cooling water released

20 have been made by comparing three specific sites in the appendices - Windscale,

21 and suspended solids. The oceans are always in motion, the scale of movement ranging from Brownian movements

22 The waters of the open-ocean are more stably stratifi- continental shelf. ed than those

23 3.3.1 Hydrogen-3 (Tritium) H is released into the coastal environment from both nucle- Although ar power

24 strontium, as one of the major dissolved constituents in sea water. some processes calcium acts very similarly In

25 other principal fission products. Iodine nuclides are,

26 After the dissolution of spent fuels with nitric acid 106 Ru in the acid solution

27 Because of the fact that the chemical speciation of 106 Ru in sea water is so much dependent on the condition and history of the released effluents, its behaviour in the coastal environment is not fully understood with respect to its speciation equilibria. It has been observed, however, that ^

28 As stated,

29 'solution' consists primarily of Pu (V + VI), and that the K^ values for this pair

30 redistributed within and/or released from settled sediments. is This topic

31 which are considered to be essential for the functioning of normal metabolic processes. Trace elements

32 A useful source

33 must be a composite of these, and similarly that k represents all routes of excretion. There is considerable experimental evidence, however, that radionuclides accumulated direct from sea water by marine fauna may have a different tissue distribution,

34 the rate of discharge to the filtered seawater concentration, and then relating this value in turn, to a concentration factor based on filtratederived data.

35 ments, particularly for multivalent cations, although it has also been observed that a number of metals are incorporated into various forms of granules - probably as a means of detoxification - which may or may not be subsequently excreted. Crustaceans, which grow by a process of moulting,

36 employed, successfully, to estimate the probable concentrations of radionuclides

37 for diverse food chains (Thomann, 1981).

38

39 As to be expected, there have been many studies on the accumulation of Sr by fish, the most recent review of which is that of Pentreath (1977). Environmental samples have been analysed from the Pacific proving grounds, the Atlantic and Indian oceans, the Black Sea, the Caspian Sea and

40 by Pentreath (1977)

41 4.3.6 Zirconium-95/Niobium-95 Concentrations of Zr and Nb, usually measured collectively, indicate

42 be superfluous. By and large the concentration factors observed for algae, invertebrates

43 have produced further data

44 5. HABIT SURVEYS AND CRITICAL GROUPS

45 of a critical group dose assessment should not be unduly influenced by the habits of a particular individual; indeed ICRP-7 (1965) states that 'dramatically unconventional 1 observations

46 With regard

47 clear that whereas data to a reasonable degree of accuracy are required when estimating radiation exposure

48 The IAEA has a general responsibility for developing standards, and advising on regulations to control the extent of aquatic pollution by radioactive materials,

49 critical review

50 AVARGUES, M., et al. (1968). des radionucléides Recherches expérimentales sur l'accumulation

51 BROECKER,

52 CLIFTON, R. J, et al. (1983). radionuclides present Concentration and depuration of some

53 FISHER,

54 GUARY,

55 HARVEY,

56 HUNT,

57 I.A.E.A. (1978). The Radiological Basis of the IAEA Revised Definition and Recommendations Concerning High-level Radioactive Waste Unsuitable for Dumping at Sea. IAEA, TEC. DOC. 211, Vienna, 58 pp. I.A.E.A. (1979a). Behaviour

58 ICRP (1980), Limits for Intakes of Radionuclides by Workers. (Annal. ICRP 4(3/4)), ICRP Publ.30, PL.2, Pergarnon Press, Oxford,

59 KECKES, S., et al. (1967). physico-chemical forms Accumulation of electrodialytically separated

60 MARTIN, J.-L. M. (1972). Etude de l'absorption, de le concentration et du métabolisme du strontium 85 chez le crustace decapode Carcinus maenas. Mar. Biol., 12: MASSON, M., et al. (1981). transferts Approches expérimentales de l'étude des

61 NELSON, D. M., LOVETT, M. B. (1981). Measurements of the oxidation state and concentration of plutonium in interstitial waters of the Irish Sea. IAEA-SM-248, Vienna, IAEA, Vienna, (STI/PUB/565). NELSON, D. M., ORLANDINI, K. A. (1979). Identification of Pu(V) in natural waters. Argonne National Lab., Argonne,

62 PENTREATH,

63 PRESTON, A., JEFFERIES, D. F. (1967). The assessment of the principal public radiation exposure from, and the resulting control of, discharges of aqueous radioactive waste from the UKAEA factory at Windscale, Cumberland. Hlth Phys., 13: PRESTON, A., JEFFERIES, D. F. (1969a). Aquatic aspects in chronic and acute contamination situations. IAEA-SM-117, Vienna, IAEA, Vienna, (STI/PUB/226). PRESTON, A., JEFFERIES, D. F. (I969b). The I.C.R.P. critical group concept in relation to the Windscale sea discharges. Hlth Phys., 16: PRESTON, A., MITCHELL, N. T. (1973). Evaluation of public radiation exposure from the controlled marine disposal of radioactive waste (with special reference to the United Kingdom). IAEA-SM-158, Seattle, IAEA, Vienna, (STI/PUB/313). RAI, D., et al. (1980). Solution species of plutonium in the environment. J. Environ. Qual., 9: RILEY,

64 SANTSCHI, P. H., et al. (1979). Natural radionuclides in the water of Narragansett Bay. Earth Planet, Sei. Lett.,

65 TEMPLETON, W. L., PRESTON, A. (1966). radioactive effluents Transport and distribution of

66 WOODHEAD,

67 Annex 1 RADIOACTIVE DISCHARGES FROM SELLAFIELD (UK) R. Jan PENTREATH Ministry of Agriculture, Fisheries and Food, Directorate

68 SS TT UU VV WW XX YY ZZ

69 1960

70 plant (SIXEP) comes into operation

71 pond water effluents retained

72

73 55' Sediment Nature : Irish Sea 53' Fig. 1.6 Map of the Irish Sea, indicating distributions of surface sediments expressed as % by weight of sediment <62.5 \im. Based largely

74 TABLE

75 4. BEHAVIOUR OF RADIONUCLIDES IN SEA WATER The distribution of the most soluble radionuclide, 3 H, has been studied

76 Fig. 55

77 Fig.

78 55' Pu seawater 54' Fig Concentrations of 239/240p u ^mbq i i) i n filtrate, surface waters of the Irish Sea in April From Pentreath et al., 1984, The concentrations of 23 9 /2 40p u anc j 241^ in Xrish Sea water differ from year to year. Data for filtrate surface water in 1979 are shown in Figs & 1.11 (Pentreath et al., 1984). The overall pattern of distribution is not dissimilar from that of previous years (Hetherington et al., 1975), The transuranium nuclides are also transported into the North Sea, and their distributions in total sea water samples have been described in a number of recent papers (Murray et al., 1978, 1979; Kautsky

79 55' Am seawafer 54 Dublin 53' Fig Concentrations

80 TABLE

81 TABLE 1.5 Estimates of fission product K, values (from Jefferies, 1968) Radionuclide Surface silt 95 Zr/ 95 Nb 106 Ru 137 Cs

82 fraction of the total in the sea water (Pentreath et al., 1984). If it is assumed that this body of water resides in the area with a half-time of about one year, then the quantity leaving per year can be estimated and compared with the quantities discharged in the preceding twelve months. There

83 Fig Estimated quantities (kbq m~ 2 ) of 239/240p u i y i ng within the top

84

85 As to be expected, the transuranium elements have also been examined

86 major gamma-emitting fission products were recorded in a large range of benthic algae, invertebrates and fish, and some concentration factors were calculated

87 (Pentreath, 1975) and on the relative importance of food and water in the maintenance

88

89 cribe

90 TABLE 1.8 Preliminary concentration factor data for transuranium nuclides in the Irish Sea, calculated relative to filtrate «0 = 22 p.m) sea water. These data were derived from

91 7. ENVIRONMENTAL MONITORING, SURVEILLANCE. AND ASSESSMENT OF RADIATION EXPOSURE OF THE PUBLIC

92 The highest external dose-rate estimate for the Ravenglass estuary was 11% of

93 TABLE 1.9 Maximum exposures, as a % of ICRP-9 limits

94 TABLE 1.10 Individual radiation exposures due to consumption of Irish Sea fish and shellfish, From Hunt (1983). Exposed population Consumers

95

96 CT\ TABLE 1.11 Collective effective dose equivalents from Cs in edible fish: Waters, North

97 TABLE 1.12 Collective effective dose equivalents from Waters, North Sea Cs

98 ambient sea water concentrations off Sellafield, the dose rates to developing embryos were calculated using modelling techniques. It was concluded that in view of the ß and v irradiation dose rates being less than that from natural background

99 The dose rates to the gonads of adult plaice have also been studied (Woodhead, 1971, 1973 (a), (b), 1974; Pentreath

100 ASTON,

101 CLIFTON, R. J., HAMILTON, E. I. (1982). The application of radioisotopes in the study of estuarine sedimentary processes. Estuar. Coast. Mar. Sei., 14: CRONAN, D. S. (1969). Recent sedimentation in the central north-eastern Irish Sea. Inst. Geol. Sciences, Report 69/B,

102 HEAPS, N. S. (1974). of Development of a three-dimensional numerical model

103 HOWARTH,

104 I.A.E.A. (1976). Ecosystems. Effects of Ionizing Radiation on Aquatic Organisms and Tech. Rep. Ser. No.172, IAEA, Vienna,

105 KNIGHT, A., et al. (1980). An air monitoring programme in the environment of a major nuclear establishment: operation and results. Proc. 5th Int. Congr. IRPA Jerusalem 1, LEONARD,

106 MITCHELL,

107 NELSON, D. M., ORLANDINI, K. A. (1979). Identification of Pu(V) in natural waters. Argonne National Lab., Argonne, II, ANL-79-65, Pt.III, PANTIN,

108 PENTREATH, R. J. (1981a). of transuranium The biological avaialbility to marine organisms

109 PRESTON.

110 THOMPSON,

111 Annex

112 Figure

113 2. LES RADIONÜCLEIDES REJETES

114 Tableau 2.1 Activités annuelles des différents radionucléides rejetés de 1966

115 Figure

116 Dans l'eau de mer, il se produit un réarrangement de la structure des complexes selon deux réactions concurrentes : hydrolyse et formation

117 directions dominante

118 Cap

119

120 Figure 2.6 Trajet d'un flotteur lesté lâché 2 heures avant la pleine

121 Cap

122 4.2 Etudes postérieures à la mise en service des installations Pour suivre les grandes lignes des transferts dans l'environnement de radionucléides à partir de l'émissaire de rejet de l'usine de traitement de La Hague, certains émetteurs gamma sont particulièrement intéressants : ainsi le 144 Ce est un marqueur des mouvements de la matière en suspension alors

123 Le 137 Cs, généralement très étudié, représente un élément de comparaison intéressant entre

124 Figure 2.8 Repartition géographique des sites étudiés le long du littoral de la MANCHE [GUEGUENIAT, AUFFRET, BARON (1979)]. Dans

125 dans

126 CP 10 u a tu ' 0,1

127 1 10 u a U!.- p -U "* o o LU ce LU 1 v/t LU 1.' ] < L 0,1

128

129 Fucus serra rus x Fucus vestcuiosus A Fucus spiralîs

130 Fucus scrratus x Fucus vesiculosus A Fucus spiralis

131 Tableau 2.4 Niveaux

132 Tableau

133 Des renseignements plus détaillés sur les mesures de transuraniens effectués

134 Tableau 2.7 Radioactivité massique

135

136 PECHE COTIEREC2) _^»_ LIMITE DES EAUX RESERVEES BRITANNIQUES t

137 cartographie régionale des niveaux de concentration normes pour un rejet unitaire fut établie (fig.2.7 ) afin d'évaluer les conséquences sanitaires

138 coquilles Saint-Jacques). Les tonnages sont de l'ordre de 15 tonnes par an dans la partie ouest de la côte, de Vauville au cap de La Hague et de l'ordre de 180 à 200 tonnes par an dans la partie nord du cap de La Hague à Cherbourg. Ils comprennent 75 à 80 % de poissons, 15 à 20 % de crustacés, 5 à 10 % de mollusques. Le temps de présence en mer et de manipulation des engins de pêche par un pêcheur a été évalué à heures par an en moyenne [CEA (1965 a)] Les prati_ques de_^a_pêche_à_p_i_ed En

139 Ces études générales sont complétées par des travaux plus spécifiques, tels ceux liés

140 L'étude prévisionnelle

141 AUSSET

142 FRAIZIER

143 GUEGUENIAT

144 KAUTSKY (1973) The distribution of the radionuclides caesium 137 as an indicator for North

145 Annex 3 RADIOACTIVE DISCHARGES FROM TROMBAY-BOMBAY, INDIA Bhupendra PATEL, Shakunt PATEL Health Physics Division, Bhabha Atomic Research Centre, Tombay, Bombay, India

146 Research Laboratory MAHigh Altitude Research Laboratory QHeavy Water Plant Power Station Saha Institute of Nuclear Physics ^ )Variable Energy Cyclotron Uranium Corporation

147 The distribution of these radionuclides in the local ecosystem - water, salt, silt, sediment, fish and shell-fish - from the discharge zone to a distance of about 10 to 100 km due north and south have therefore been monitored from 1967

148 from the mainland on the east. The Dharamtar Creek, at the head of which is the Amba River, enters the bay from the southeastern side. At the head is the Thana creek, lined by mud banks at low water, through which opens

149 1972; Bhat

150 9 II II il 12 I2Ï4567 Month Fig.3.4 Temporal variations in concentration of ccsium-137 in Anadara granosa (a)

151 4.2. Salt Strontium-90

152 TABLE 3.3. Distribution of cesium-137 in the suspended silt from the bay waters during (Annual average KBq.Kg" 1.)* Cesium-137 KBq.Kg" 1 silt Year 2-4 Km North Discharge zone 2-4 Km South *(1 Bq = pci) TABLE

153 sequence

154 TABLE

155 TABLE 3.8 Distribution pattern (Maximum-Minimum)

156

157 predominantly controlled ig.3>.6 Distribution pattern ofcesium-itf (pdjg dry) in surface sediment during

158 Fig.3.7 Bombay harbour

159 10 E/2 S I0 er œ E 10* 30

160 during

161 lower concentrations to the region under study. Notwithstanding these mechanisms, the desorption of some radionuclides (cesium-137, zinc-65, cobalt-60) from the sedimentary particles has been observed under laboratory conditions, with sufficient concentrations

162 ON to TABLE 3.10 Mineral composition, grain size, base exchange capacity

163 explained

164 TABLE 3.11 Range of concentration factors (Cf)* observed for cesium-137 in the flesh of various species of fish and shell fish from the Bombay harbour during Species Cf Bivalves Blood clam Anadara granosa Oyster Crassostrea cucullata Windowpane oyster Placenta placenta Clam - Paphia malabarica Clam - Meretrix meretrix

165 (

166 TABLE 3.12 Temporal variation

167 C n = F[RD n (Rf) 2 D n _ 2 + (Rf) 3 D n _ 3 where c r represents activity found F f R

168 population, is different from the other two nuclides. It is also interesting to note that although the transfer fractions of cesium and ruthenium from the water

169 ZONE

170

171 TABLE 3.15 Distribution of Cerium-144, rutheniura-106 and cesitun-137 (pci g~^ dry wt) in various tissues of Anadara granosa population from Trombay clam

172 TABLE 3.16 Distribution

173 6.4. "Ecological half-lives"

174 100 U) D W Cf) û o> - Ce-T E/2 ~060Y 1971 I I I A I

175 compartments in equilibrium with the environment, as seen from the flux patterns recorded

176 TABLE 3.18 Rate of clearance of water and electrophoretic mobility of erythrocytes of arcid clam Anadara Kranosa on exposure to contaminated sediment.

177 7. IMPACT ON THE ENVIRONMENT 7.1. Effects on marine species

178 colour of the outer layer of shell (periostracum) in the Trombay population

179

180 GANAPATHY S., PILLAI K.C. and GANGULY A.K. (1968) Adsorption

181 PATEL

182 PILLAI K.C.

183 DISPOSAL RELEVANT IAEA PUBLICATIONS

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