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211238401.Pdf https://theses.gla.ac.uk/ Theses Digitisation: https://www.gla.ac.uk/myglasgow/research/enlighten/theses/digitisation/ This is a digitised version of the original print thesis. Copyright and moral rights for this work are retained by the author A copy can be downloaded for personal non-commercial research or study, without prior permission or charge This work cannot be reproduced or quoted extensively from without first obtaining permission in writing from the author The content must not be changed in any way or sold commercially in any format or medium without the formal permission of the author When referring to this work, full bibliographic details including the author, title, awarding institution and date of the thesis must be given Enlighten: Theses https://theses.gla.ac.uk/ [email protected] RADIONUCLIDE MOVEMENT AND GEOCHEMISTRY IN INTERTIDAL SEDIMENTS IN SOUTH WEST SCOTLAND YOUSEF ALI BEN-SHABAN BSC HSc Scottish Universities Research and Reactor Centre presented as a thesis for the degree of Doctor of Philosphy in the University of Glasgow November 1989 ProQuest Number: 11007365 All rights reserved INFORMATION TO ALL USERS The quality of this reproduction is dependent upon the quality of the copy submitted. In the unlikely event that the author did not send a com plete manuscript and there are missing pages, these will be noted. Also, if material had to be removed, a note will indicate the deletion. uest ProQuest 11007365 Published by ProQuest LLC(2018). Copyright of the Dissertation is held by the Author. All rights reserved. This work is protected against unauthorized copying under Title 17, United States C ode Microform Edition © ProQuest LLC. ProQuest LLC. 789 East Eisenhower Parkway P.O. Box 1346 Ann Arbor, Ml 48106- 1346 LIST OF CONTENTS Page List of Tables iv List of Figures viii Acknowledgements xiii Abstract xiv Aims of the Project xv 1 INTRODUCTION 1.1 Radioactivity and radioanalytical methods 1 1.1.1 Radioactive decay 1 1.1.2 Equations of radioactive decay and growth 4 1.1.3 Interaction of radiation with matter 11 1.1.4 Radiation detection methods 22 1.1.5 Chemical separation and source preparation techniques in alpha spectroscopy 48 1.2 Intertidal sediments and flood plain deposits 65 1.3 Radionuclides in the marine and coastal environment 83 1.3.1 Introduction 83 1.3.2 General occurrence and distribution of natural radionuclides in the marine and coastal environment 84 1.3.3 Uranium and thorium geochemistry 88 1.3.4 210Pb geochemistry 98 1.3.5 Applications of natural decay series nuclides to the study of coastal and marine processes 101 1.3.6 Geochemistry of the rare earth elements 119 i 1.3.7 Manmade radionuclides in the coastal and marine environments 124 1.3.8 Applications of manmade radionuclides as tracers of environmental processes 171 2 EXPERIMENTAL 2.1 Sample collection and pretreatment 179 2.1.1 Ardmore Bay 179 2.1.2 Skyreburn Bay 180 2.1.3 Surface intertidal sediments 180 2.1.4 Flood plain deposits 182 2.2 Instrumental analytical methods 184 2.2.1 Direct gamma spectroscopy analysis of sediment samples 184 2.2.2 Neutron activation analysis 193 2.3 Radiochemical analyses 201 2.3.1 210Pb analysis 205 2.3.2 Plutonium analysis 2 07 2.3.3 Uranium/thorium analysis 210 2.4 Sequential leaching of uranium 214 2.5 Alpha particle track studies 217 3 RESULTS 220 4 DISCUSSION 271 4.1 Ardmore Bay 271 4.2 Transport processes affecting manmade radionuclides in intertidal sediments in south west Scotland 278 4.3 Skyreburn Bay 296 4.4 Netherclifton Merse: supply mechanism, inventory and surface sediment concentrations of Sellafield waste radionuclides 315 ii Page 4.5 The vertical distribution of Sellafield waste radionuclides in flood plain and intertidal sediments at the Netherclifton site 324 4.6 Natural decay series radionuclide studies at the Netherclifton site 336 4.7 Sellafield waste radionuclide studies at the Wigtown Martyr's Stake merse site 346 4 .8 Stable element geochemistry studies in Netherclifton and Wigtown Martyr's Stake merse section samples 358 4.9 Conclusions 365 References iii LIST OF TABLES Table Number Page 1.1 Decay characteristics of radionuclides of interest in this study 5 1.2 Ionic potentials for selected elements 91 1.3 Natural decay series radionuclides which can be used in chronology studies 108 1.4 Radionuclides in weapons testing fallout 127 1.5 Discharge data for Chapelcross and Hunterston 136 1.6 Quantities and activity ratios of selected nuclides discharged as low level liquid effluent from Sellafield in the period 1957 to 1987 137/9 1.7 Kp values for selected elements 150 1.8 Radionuclide activity ratios for possible sources of contamination of Solway Firth intertidal sediments 159 1.9 MAFF estimates of critical group exposures as a result of the Sellafield liquid effluent discharge 168 1.10 Radionuclides detected in rainwater in south west Scotland (6 May 1986) as the result of Chernobyl fallout 170 2.1 Typical calibration of the 80cc Ge(Li) detector using 226Ra as a standard source 188 2.2 Analytical data for calibration of the detection efficiency for 134Cs, 137Cs and 241Am direct 7 spectroscopy for sources of varying height and composition 191 2 . 3 Analytical data for 15 repeat analyses of a single sample of silt for 137Cs and 241Am by direct 7 spectroscopy 192 2.4 Results for 15 repeat analyses of a bulk silt for 137Cs and 241Am by direct 7 spectroscopy 194 iv Table Number Page 2.5 Irradiation and counting data for neutron activation analysis 199 2 . 6 Observed concentrations (derived by INAA) and IAEA reference values for SOIL 5 202 2.7 Observed concentrations (derived by INAA) and IAEA reference values for SOIL 7 203 2 . 8 a Analytical data for assessment of the precision of the plutonium analysis by replicate analysis of a bulk sample of Solway silt 211 2 .8 b Analysed data and reference values for analysis of IAEA standard sediment for plutonium 211 2.9 Analytical results for uranium and thorium analysis of reference sandstone DL-la along with CANMET certified values 215 3.1 210 Pb concentrations• m• samples from three cores of Ardmore Bay intertidal sediment, March 1984 221 3 . 2 Radiocaesium and dry weight/wet weight results for core ABC871 from Ardmore Bay, July 1987 223 3 . 3 Radionuclide concentrations and activity ratios in surface intertidal sediment samples from various locations in south west Scotland 225 3.4 Neutron activation analysis results for surface intertidal sediment samples from various locations in south west Scotland 226/7 3.5 Radionuclide concentrations and activity ratios for samples from Skyreburn Bay intertidal core SBC831 228 3 . 6 Radionuclide concentrations and activity ratios for samples from Skyreburn Bay intertidal sediment core SBC851 231 3.7 Radionuclide concentrations and activity ratios for samples from Skyreburn Bay intertidal sediment core SBC852 233 3.8 Radionuclide concentrations and activity ratios for samples from a surface transect, Netherclifton, March 1985 235 v Radionuclide inventories in merse silt samples, Netherclifton, August 1987 (a) 0-15cm, (b) 15-30cm and (c) 0-30cm 239 Radionuclide concentrations and activity ratios for samples from section NCS861, Netherclifton 240 Radionuclide concentrations and activity ratios for samples from core NCC861 , Netherclifton 243 Radionuclide concentrations and activity ratios for samples from section NCS862, Netherclifton 245 Radionuclide concentrations and activity ratios for samples from section NCS863, Netherclifton 248 Radionuclide concentrations and activity ratios for samples from section NCS864, Netherclifton 249 Natural decay series radionuclide concentrations and activity ratios for surface soil samples from a 55m transect, Netherclifton 250 Uranium and thorium concentrations and activity ratios for selected samples from Netherclifton merse sections plus a sample of surface silt from the north eastern basin of the Irish Sea 252 Uranium association with different soil fractions from Netherclifton merse and intertidal sections 253 Alpha particle track density produced in CR-39 plastic by a sample from section NCS862, Netherclifton 254 Radionuclide concentrations and activity ratios for samples from a 500m surface transect, Wigtown Martyr's Stake (a) 0-15cm depth and (b) 15-30cm depth 255 Dry/wet weight ratio, % loss on ignition and fraction of silt of size <75/m data for the Wigtown Martyr's stake 0-15cm samples 256 vi Table Number Page 3.21 Radionuclide inventories for samples from the Wigtown Martyr's stake transect (a) 0-15cm, (b) 15-30cm and (c) 0-30cm depth 261 3.22 Radionuclide concentrations and activity ratios for samples from section WMS871, Wigtown Martyr's stake 264 3.23 Radionuclide concentrations and activity ratios for samples from a section cut into an exposed vertical face of merse deposit at depth 5cm, Wigtown Martyr's stake 267 3 .24 Radionuclide concentrations and activity ratios for samples from a section cut into an exposed vertical face of merse deposit at depth 75cm, Wigtown Martyr's stake 267 3.25 Neutron activation analysis results for merse silt samples (a) Netherclifton and (b) Wigtown Martyr's stake 269/70 4.1 Summary of radionuclide concentrations and activity ratios reported for Solway intertidal sediments 282 4.2 Summary of previous radiocaesium results for Skyreburn Bay intertidal sediment profiles (A B MacKenzie, Pers. Comm.) 297 4.3 Radionuclide concentration correlation coefficients for samples from section NCS862 (a) 0-50cm, (b) 50-100cm and (c) 0-100cm 329 4.4 Excess concentrations relative to Irish Sea silt for the
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