Study of radionuclides, lead and lead isotope ratios in Scottish sea loch sediments
Shimmield, Tracy Marjory
This research involved the study of sediment cores from Loch Etive, Loch Long, Loch Goil and Loch Fyne with the aims of investigating the geochemistry of natural, and manmade radionuclides and heavy metals within the sea loch environment. The main aims of the research were to determine accumulation rates and the extent of mixing within these sediments and to assess the fluxes, sources and temporal variations in input of pollutant heavy metals to these environments. In recent years it has been suggested that Pb is mobile in sea loch sediments which questions the validity of applying ²¹⁰Pb dating in this environment. This has important implications with respect to interpreting sediment cores to assess temporal trends of pollutant inputs and investigating the rates of physical and biogeochemical processes that are taking place in the coastal environment. Hence, one of the aims of this research was to determine whether Pb was mobile in these sediments. The ²⁰⁶Pb/²⁰⁷Pb isotope ratio can potentially be used to determine the extent of pollutant Pb input from leaded petrol to the environment and a further objective of the work was to investigate the isotopic signature of pollutant Pb in the sediment. Concentration of ²¹⁰Pb, ²²⁶Ra, ²²⁸Ra, ²²⁸Th, ²³⁸U, ¹³⁷Cs, ¹³⁴Cs and ²⁴¹Am in the sediments were analysed using gamm a spectroscopy and the heavy metals, Pb, Zn and Cu were determined using X-ray Fluorescence. Stable Pb isotope ratios were determined using Inductively coupled plasma Mass spectrometry. The results obtained indicated that Pb is not subject to diagenetic mobility in these sediments and that ²¹⁰Pb profiles can be used to determine sedimentation rates for most of the sediment cores. lt was not possible to determine accumulation rates for the two cores from Loch Fyne by ²¹⁰Pb dating, and in this case the sedimentation rate was assessed by correlating the maximum concentration of ¹³⁷Cs in the sediments with the maximum ¹³⁷Cs discharge from Sellafield, BNFL's reprocessing plant located on the Cumbrian coast. The flux of ²¹⁰Pb to the lochs varied significantly suggesting that there has been sediment focusing of fine and/or organic rich material to the deeper sites, resulting in an enhanced flux of ²¹⁰Pb to these sediments. Sellafield waste radionuclides also provided useful chronologies by relating sediment maximum concentrations to maxima in the discharges. ¹³⁷Cs was observed to be subject to diffusive movement, invalidating the use of its total depth of penetration as a chronological indicator. The temporal trends of pollutant metal input agreed well with known historical trends and the Pb isotope profiles indicated that the onset of deposition from pollutant Pb from petrol occurred in the late 1920's. The maximum input of Pb from petrol peaked in the early 1980's and since then there has been a decrease in this input. The two sea lochs which were closest to the industrial centre of Glasgow exhibited a large anthropogenic pollutant input, confirming that these sediments have been highly perturbed by human activities, either directly as a result of sludge dumping or due to changes in land use (eg. road construction, deforestation, etc.) in the catchment. All the sea lochs reflected a change in the supply of material to the sediments over the last eighty years, indicating that increased anthropogenic activity has had an effect on these environments.