IAEA-TECDOC-481 INVENTORIES OF SELECTED RADIONOCLIDES

Transcription

1 IAEA-TECDOC-481 INVENTORIES OF SELECTED RADIONOCLIDES

2 INVENTORIES OF SELECTED RADIONUCLIDES IN THE OCEANS IAEA, VIENNA, 1988 IAEA-TECDOC-481 ISSN Printed by the IAEA in Austria October 1988

3 In March 1984 FOREWORD

4 EDITORIAL NOTE In preparing this material for the press, staff of the International Atomic Energy Agency have mounted and paginated the original manuscripts as submitted by the authors and given some attention

5 Assessment CONTENTS

6 Please be aware that all the Missing Pages in this document were originally blank pages

7 ASSESSMENT

8 dynamics of oceanic carbon and its updates exchange with the atmosphere, and

9 It

10 so must

11 The effect upon this estimate of including biospheric exchange is small since returning carbon fluxes

12 there

13 Table 3.1 INVENTORIES OF BOMB ^C IN THE ATMOSPHERE (in atoms of Bomb Stratosphere 2 Troposphere 3 Year yield (Mt) 1

14 Bomb

15 changes; and to Investigate large-scale oceanic transport and mixing processes. Measurements pertinent to radiocarbon determinations (including 6 13 C, 6 ltf C values and DIOC concentration) embrace only a few

16 Lü O TOO " PRE-BOMB A I4 C V N PACIFIC *- -* S PACIFIC «- * N ATLANTIC

17 4.1.4 "Radiocarbon

18

19 The relative shallowness

20 PRE-BOMB RADIOCARBON RESULTS X_J*-**->& -20 -jo WA -70 x Atmosphere (Irees) a Ftorido coral Almospheit (Irees) Beim cord -90 Btimudo coral o Golo'poijos axol -100, 800

21 Killough and Emanuel (** 3 ) have assembled a pre-industrial record from sources cited above. A surface value of A^C 0 = -40 / 00 is assumed in preference

22 TOTAL

23 Atlantic Table 4.1

24 water mass (1.38xl0 9 )

25

26 Fig. 4.7:

27 Table 4.2b Bomb-carbon Summary for Individual Ocean Regions Showing Either Excess or Deficient Inventories Relative

28 INPUT AS OF GEOSECS SURVEY Fig. 4.8: Ratio of water column inventory to net input of bomb radiocarbon for the stations occupied during the GEOSECS program. The ratio averaged over each

29 4.3.7 Oceanic inventories

30 are largely confined

31 Although a consensus of both cosmogenic and bomb-carbon inventories seem evident from table 4.3,

32 discernible decline at all, since the early 1970s, but do indicate strong seasonal effects

33 abundance of these ions vary with temperature and pressure and thence with depth. Typical profiles of [DIOC] are displayed in figs 5.1 and 4.6. Table 5.1 records the estimated depth structure of DIOC TALK {/ieq/kg) Fig. 5.1: The mean vertical distribution of (a) the alkalinity ("TALK") and (b) the total DIOC concentration ("TC0

34 Table 5.1 Oceanic inventory

35 Thus, ignoring minor constituents, [Alk]

36

37 Stuiver( 6 ) analysed radiocarbon data from 6EOSECS Atlantic stations, and deduced

38 Local exchange rates are expected to be proportional to the partial pressure in the departing medium. Invasion rates will therefore have increased

39 (b) Stuiver( 7 ): Stuiver summarises available estimates

40 Table

41 5.4 Models of the Global Carbon Cycle

42 In numerically implementing box-diffusion models to study carbon dynamics, Oeschger found it appropriate to stratify the diffusive reservoir into a finite number (viz, 42) of layers. Several recent models have explicitly incorporated a multi-box structure in an attempt

43 equally good accounts

44 The integral over A 1 '*C* a -j r is determined by noting that the post atmospheric record (fig. 3.1)

45

46 ACKNOWLEDGEMENT

47 15 Manning, M.R., Jansen, H.S., McGill, R.C., and Burr, M.K., "A summary of atmospheric carbon 14 measurements made in the South Pacific from 1954

48 Gordon, A.L., "Interocean exchange of thermocline water", J. Geophys. Res., 91, , Nozaki, Y., Rye, D.M., Turekian, K.K. and Dodge, R.E., "A 200 year record of carbon-13 and carbon-14 variations in a Bermuda coral", Geophys. Res. Lett.,

49

50 71 72 Kanwisher, J., "On the exchange of gases between the atmosphere and the sea", Deep-Sea Res., 10, , Wannikhof, R., Ledwell, J. and Broecker, W.S., "Gas exchange -wind speed relation measured with sulfur hexafluoride

51 INVENTORY OF 137 Cs AND ""Sr IN

52 In what follows the input from runoff is assumed to be 3X of fallout input ( i5 > 25> 27 ) unless specific information is available (e. g. the Baltic< 45 > ). Information

53 Table _!_. S_. Atlantic 137 Cs inventories by latitude band. Latitude band O-1O S 1O-2O S 2O-3o S 3O-4O S 4O-5O S 5O-6O S 6O-7O S 7O-OO S Geosecs inventory (PBq) , Fallout inventory (PBq) Total inventory 28. 4^5, 4 PBq Sediments: estimated

54 of water is much shallower than the oceans discussed, thus far, and the waters

55 50 30 \*** <->;/> ; ^ * N <& FIG.1.

56 Overall

57 9. S. Pacific Very

58 further north;

59 11. North Sea Tills sea was not covered in the previously cited paper on the K. Atlantic, but is particularly important because it is greatly affected by the effluents from the Sellafield and Cap La Hague reprocessing plants and is a contributor to other seas further north. The inventory question is covered in great detail in the accompanying paper

60 Bq km" 2, which with an area of E6 Km 2 gives an inventory of O,

61 translatable to a 137 Cs value) and some results for tue Barents Sea by Kautsky (^J. It is possible to take the latter and attempt to calculate

62 et al. ( 1Q ) do not quite coincide for the vicinity of Svalbard, that of Kautsky being longer, though relying

63 earlier

64 Table 5. i37 Cs Inventories for al 1 world oceans. Ocean N. Atlantic S. Atlantic Caribbean Mediterranean BlacK

65 (1) Aarkrog, REFERENCES

66 (11) Domanov, M. M. and Nelepo, B. A. (1975). Study of the structure o± cesium

67 (22) Kautsky,

68 (34) MiyaKe, Y, and Sugimura, Y, (1976). The Plutonium content of Pacific Ocean waters,

69 (45) Salo, A., Tuomainen, K. and Voipio, A. (1902). The inventories of certain long-lived radionuclides in the Baltic Sea. in "Transuranic cycling behaviour in the marine environment" IAEA-TECDOC-265,

70 ARTIFICIAL RADIOACTIVITY IN THE NORTH SEA AND THE NORTHERN NORTH ATLANTIC DURING

71 those

72 The large-scale distributed measurements permit the calculation of balances of the total content

73 4.2 Northern North Atlantic Almost the whole of the Caesium introduced into the sea with the waste waters of the Sellafield Works

74 the North

75 one considers the data from the different regions then one can see the following mean transport times from the Sellafield Works to the respective regions: Southern Norway

76 At the few stations in the Barents Sea where water samples have been taken from the surface and from 100m depth, the ratio values of

77 9. FIRST MEASUREMENTS AFTEK THE ACCIDENT AT CHERNOBYL (25) Via the fallout and the precipitation, artificial radionuclides - which were emitted into the armosphere from the accident at Chernobyl - entered the North Sea surface water

78 The vertical distribution of the 137 Cs shows, as is to be expected, seasonally conditioned differences. However, effects also occur, which - on the basis of the data available

79 Further particular thanks are extended to Mrs.fetersitzke for the intensive work on the translation of the original German manuscript, as well as the Deutsches Hydrographisches Institut for the kind permission to use freely the material available - particularly

80 (21) BONI,A.L., 1966 : Rapid ion exchange analysis of radiocaesium in milk, wine, seawater, and environmental samples. Analytic.Chem.

81 Estimation Table 2

82 UMiem Table S»

83 Tible 5b Content of»sr fa, the witer of (he North Sf«during 1»79 Region 51

84 Table 6 Annual dischargee of 15^Cs and 157 Cs (TBq «y~ 1 ) from

85 Table 8 Activity concentrations of Cs and Cs and their ratios at three positions

86 Table 11 Activity concentrations of Cs and Cs and their ratios in the water

87 r^, 'Pttmovlltf]^* Southwnpwn

88 Dischorge Sellofield Works dito 137 Cs*V 2 13t Cs-.» Sr PentlondFirlh58HO'N02 E 50'W 55* 30'N 06'E o î. I/I LJ J m B o X--'"''»" V \ - - -' "o « " ear ** 1984 Fig

89 Fig. 137+W Cs in surface water February/March

90 U- Cs Pig. 5

91 Fig. 6 or near bottom down to 85m depth Apr il/ June

92 33 u3l,,35 surface 50m or near "bottom 100m or near bottom 250m

93 90 Sr Pig. 8

94 «s' Fig Pu. 238 un surface water Pu' August/September

95

96 ^>> cs r A. Tritium Pig.11

97 89 Pig.

98 (800) II Su»fa«50«00 M 250m vrnear bottom 00m 750m 1000m 1250m 1500m 2000«1500 m Pig.

99 Ratio Pig.14-

100 Aug.-Sept.1979

101 Pig.16 1^'Cs in the water (Bq.m ) Figures

102 WORLDWIDE DATA ON FLUXES OF»» «Pu AND 238 Pu

103

104 Table 2.2. Atlantic Ocean Areas Latitude Area in 10 6 km 2 > 30 N 35 N-Atlantic

105 In the Northern Hemisphere the integrated deposition density of 239,240 Pu i s 39 Bq m-2 an<j i n tne southern it is found to be 9.7 Bq m~2

106 Table Expected 239,240p u inventories from global fallout in the Atlantic Ocean Latitude band 239,240p u inventory in PBq > 3QON N S 0.24 >30 S 0.27 However besides

107 ratio

108

109 tude bands between 140 E

110 40 N

111 Table 4.2 Estimated 239,240p u inventories in latitude bands (Table 3.1.2) thé Atlantic Ocean based upon GEOSECS data (Appendix Table A.4) Latitude band > 30 N 0-3

112 239,240p u m~2.

113 We may conclude that around 50% (cf. 3.3.) of all 239,240 Pu discharged from Sellafield

114 In 1975 Bowen (1979) found

115 5. Discussion 5.1. Measured versus expected ocean inventories In the calculations of the oceanic Pu-inventories from the Geosecs data/ it has been assumed that the area deposit in the marginal seas has been the same as for the nearest Geosecs stations in

116 led

117 By using sediment traps Livingston (1983) has determined the average deep sea 239,240p u fluxes in the equatorial north-west Atlantic (13 05'N, 54 W) to Bq m~ 2 yr" 1 and in the equatorial North Pacific (15 2TN f 151 W) to Bq m~ 2 yr" 1. From this

118 tions, whereas

119 Appendix; Data used in the report Table A.1. Plutonium 239,240 inventories in Pacific water columns collected during the GEOSECS programme (Livingston, 1985a) Cruise station Position (cf. Fig. A.1) GX-201 GX-202 GX-204 GX-212 GX-214 GX-217 GX-218 GX-222 GX-223 GX-224 GX-225 GX-226 GX-227 GX-229 GX-231 GX-235 GX-239 GX-241 GX-246 GX-251 GX-263 GX

120 Table A.2. Plutonium 239,240 inventories in Pacific water columns collected during various cruises (cf. Fiqs.

121 Table A.4. Plutonium 239,240 inventories in Atlantic water columns collected during the GEOSECS Cruise station GX-3 GX-1 1 GX-1 4 GX-1 7 GX-1 9 GX-27 GX-29 GX-31 GX-33 GX-3 7 GX-40 GX-49 GX-54 GX-60 GX-67 GX-1

122 O LARGE VOLUME STATION» SMALL VOLUME STATION O SOT STATION Fig. A.1. Geosecs Pacific Expedition (Livingston, 1985a) 123

123 -700 ta 800 m ^

124 SEDIMENT

125 Il II II !l o LARGE VOUHC STATCN SMALL VO.LME STATION

126 Fig. A6. Irish Pu-concentrations in filtrate, surface waters of the

127 Global fallout ( 240 Pu/ 239 Pu-0.l8) Nevada I fallout (240 Pu/ 239 Pu =0.035) SHELF SLOPE RISE >95%of

128 Aarkrog

129 British Nuclear Fuels pic (1985). Annual Report on Radioactive Discharges and Monitoring of the Environment 1984 (and earlier years reports); Risley, Warrington, Cheshire,

130 Fowler S.W., Ballestra

131 Hayes D.W.,

132 Kupferman S.L., Mass Balance for Livingston H.D. and Bowen V.T. (1979). A

133 Livingston H.D., Kupferman S.L., Bowen V.T. and Moore R.M. (1984). Verticale Profile

134 Murray C.N. and Fukai R. (1978). Measurement of Pu in

135 Pentreath R.J. (1985). Radioactive Discharges from Sellafield (UK). Annex

136 tonium Isotopes

137 LEAD-210 AND POLONIUM-210 IN THE WORLD'S OCEANS R.D. CHERRY Department of Physics, Cape Town University, Cape Town, South Africa M. HEYRAUD International Laboratory of Marine Radioactivity, Océanographie Museum, Monaco Abstract After a brief summary of the sources of 210 Po an( j 210pjj j n t^e ocean) the published data for these two nuclides are discussed in four sections. 1. Surface sea water (^100 m) from the open ocean. 2. Surface sea water from coastal regions. 3. Depth profiles in the open ocean. 4. Data from atypical regions. Estimates of the global inventories of 210p o an( j 210pb are ma<j e and compared with the 22 "Ra inventories (Bojanowski, this volume). Over the whole water column in the three major oceans 2 10po and 2 -^pb are j n approximate equilibrium.

138 The fall-out flux

139 Other possible sources of p^ ^n t^e atmosphere are of relatively minor importance. They have been reviewed

140

141 oceanic surface waters, by all processes other than radioactive decay, is typically between

142

143 (i) Usually, the depth profiles show an activity excess of p^ OVer

144 55% over equilibrium; below that there is approximate equilibrium, source of

145 Table

146 Table III.

147 0.13,

148 Appendix REFERENCES 0, P 0, C, u 0, P 0, Bacon, M.P.: 210 Pb and 210 Po results from F.S. "Meteor" cruise 32 in the North Atlantic. "Meteor" Forsch.-Ergeb., Reihe A 19, (1977) Bacon, M.P. and A.W. Elzerman: Enrichment of 2l Pb and 210 Po in the sea-surface microlayer. Nature 284, (1980) Bacon, M.P.. D.W. Spencer and P.G. Brewer: 210 Pb/ 226 Ra and 210p 0 /210pb disequilibria in seawater and suspended particulate matter. Earth Planet. Sei. Lett. 32, (1976) Bacon, M.P., D.W. Spencer and P.G. Brewer: Lead-210 and polonium-210 as marine geochemical tracers: review and discussion of results from the Labrador Sea. In "Natural Radiation Environment III", Houston, vol. P, 0, 0, P 0, P,

149 o, Cochran, J«K., M.P. Bacon, S. Krishnaswami and K.K. Turekian: 210p o o, o, u, o, o, P u 0, P

150 0 I Nozaki, Y., J. Thomson and K.K. Turekian: The distribution of I 210 Pb

151 0, P Turekian, K.K. and Y. Nozaki: 210 Po and 210 Pb in the eastern South Pacific.

152 Data for Lead-210, Polonium-210 Inventories: Pacific Ocean Coordinates N, E

153 Data

154 Data for Lead-210, Polonium-210 Inventories: Atlantic Ocean Coordinates Bq cm" Pb 210 Po Reference

155 Data

156 Data for Lead-210, Polonium-210 Inventories: Red Sea Coordinates N, E N, E

157 INVENTORY OF RADIUM ISOTOPES IN THE OCEANS R. BOJANOWSKI Institute

158 the thorium isotopes continuously produced from uranium in the water column /73 91/. The decaying thorium atoms recoil radium nuclei to interstitial waters from which they diffuse

159 national Hydrographie Bureau./Spec. Publ. No. 23» 3nd éd., Monte Carlo, 1953/. While

160

161

162 further

163 TABLE Ra PROFILES IN THE ATLANTIC OCEAN Latitude band Coordinates H M N 60-50» 50-I»O N 1« N 30-20» 2O-1O N 1O-O N 0-10 S S 2O-3O S 30-<tO S *.0-50 S 50-6o s 6o-70 s 70-8O S «7««0 56' 63 32' l 6 02' 39 00' 38 17' 35 59* ' «, 7 ; 3Î to' 30 «if 28 «. l.' Z8 02' 27 OO' lt 6' 2 3 5o; ' 21 OO' 16 28' 16 if:!'#« ' 9 29' 3 57' 2 31' 2 00' 0 00' l«00' 5 02' 12 00' 15 03' 21 00' 2«. 00' 27 00' 32 58' «.8 39' 9 3V" 55, 1' 56,16' 57 0 «.««' 60 02* ' 70 22' 73 27' 75 52' ' 1 07' 35 IV Î8 3V l*l» 02' 69 10' «7 01' «47*00 ' 68 00' 67 21' 1

164 TABLE Ra PROFILES IN THE PACIFIC OCEAN Latitude band 1 Coor<ldLnate0 f 2 X N 50 -UO N l.0-30 N K N 1O -O M O -IO G n.3) o o S 57 00' 57 00' 53 07' r 44 4o' 44 04' 43 C4' 4l 20' 4o io' 38 35' 37>'t' ' 34 18» 34 16' 34 08' 33 03' 32 37' ' 29 5.?' X7Î «19 57' 17 Î4 Ô7' 12 53' 8 07' ' Z» 3 ''' o oo- «,«34» t+ 38* 5 01' 6 30' 1O 00* » S S '.0-50 s s Û0-70 S

165 TABLE Ra PROFILES IN THE INDIAN OCEAN Latitude band Coordinates Dapth m 226 Mean t 2 3 It 2O-10 N 19 43'N '2059' 12 30' 'E 53 16' 64 28' 84 29' 32OO 28OO 4 1OO S 0-10 S 8 31' 6 12' 5 00' 3 56' 0 01' 0 04'S 5 oo' 5 02' 6 09' 9 22' 86 03' 64 24' o 03' 50,53'E 90 45' 80 00' 9i 47' 50 55' 95 02' ( ( O S 10 OI' 12 17' 13 02' ' 17 l8 f 19 29' 79 59' 3'«39' 97 08' 79 58> S 20 06' 23 00' 24 28' 27 00' 27 04' 29 15' 79 59' ' 67 06' 56 58' ' OOO 51OO S 37 48' 33 1O' 39 57' 57 35' ' ' 54OO S 47 38' 4? 40' '57 52' s 53 00' 56 02' 57 59' 39 59' 59 I9' ' ' ' ' 92 38' S 64 o4' 64 11' 66 l4' I38 12' B3 59' '

166 TABLE 5. MEAN CONCENTRATIONS OF 226 Ra IN DIFFERENT WATER LAYERS FOR SINGLE 10 LATITUDE BANDS latitude bond n* Ra concentration in layer /Jem/ Bq m~-' «4-5 >5 0-botto» v^ 226 Bq cm ATLANTIC OCEAN K O-4O to-o Avornffe O N Û4O 1.4O S 1O-2O jo O- 8O Average Overall S «. J7 SO-50 N JO-40 ' DO-2O 2O-10 to-o Average O-1O S O O N *

167 with their respective standard deviations. When no value existed for a given strip a mean of the neighboring values was used. The sum of subinventories in each water layer yields a total inventory which is very similar to the one determined by the first method /'Table

168 Because of" the distinct features of the North Polar Ocean it was talcen apart from

169 6. RADIUM OUTPUT Radium

170 produced

171 The results are as follows: Atlantic Pacific Indian

172 REFERENCES 1. BACON,M.P., SPENCER,D.V., BREVER,P.G.

173 12. CHUNG,Y.C., "Radium-226 and Ra-Ba relationships in Antarctic and Pacific waters", Earth Planet.Sei.Lett., 23/197V « CHUNG,Y.,

174 27. FEELY.H.V., KIPPHUT,G.W., TRIER,R.M., KENT,C., " Ra and o o o Th. in coastal waters", Estuarine coast.mar.sei., 2/198O/ F0YN,E., KARLIKjB., FETTERSSON,H., RONA,E., "The radioactivity

175 KNAUSS,K.G.

176 53- LI,Y H., MATHIEU,G., BISCAYE,?. t SIMPSON,H. J., "The flux of 226 Ra from estuarine and continental shelf sediments", Earth Planet.Sei.Lett., 37/1977/ 237-2M. 5k. MIYAKE,Y., SUGIMURA,Y., TSUBOTA,H., "Content of uranium, radium

177

178 80. SHANNON, L. V., CHERRY, R. D., "Radium-226 in marine phytoplankton", Earth Planet. Sei. Lett.

179 9**. IYENGAR,M.A.R., "Distribution p rt /?

180 HOW TO ORDER IAEA PUBLICATIONS An exclusive sales agent for IAEA publications, to whom all orders and inquiries should be addressed, has been appointed in the following country: UNITED STATES OF AMERICA UNIPUB, 4611-F Assembly Drive, Lanham, MD In the following countries IAEA publications may be purchased from the sales agents or booksellers listed or through major local booksellers. Payment