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1. INTRODUCTION 1.1 the Problem the Purpose of This Work Was To

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1. INTRODUCTION 1.1 the Problem the Purpose of This Work Was To 1. INTRODUCTION 1.1 The Problem The purpose of this work was to investigate the role of aquatic plants and sediments in radium (Ra, a radioactive product of uranium) transport through the Mageia floodplain, a tropical wetiand that drains the Ranger uranium mine. To achieve this purpose, the natural Ra distribution on the floodplain was surveyed, laboratory experiments were carried out on Ra uptake by aquatic plants and sediments and the results were used to build a computer simulation model of Ra flow through the system. Experiments that could not feasibly be conducted in the laboratory or in the field were then carried out on the computer model to simulate waste water releases and to test hypotheses about the role of the plants and sediments. This approach to science is relatively new. Hut and Sussman (1987) summarised it as follows: "High-speed computation is changing the way science is done ... computational experiments ... are now becoming as important as theory, observation and laboratory experiments (because) infeasible experiments can be done and parameters inaccessible to experiment or observation can be measured ... (such) synthetic methods (are taking) their place firmly next to the traditional methods of reductionist analysis". 12 The Magela Floodplain The Magela floodplain, in the Kakadu (World Heritage) National Park, Northern Territory (Figures 1.1, 1.2), drains two large uranium deposits: Ranger, where mining began in 1980, and Jabiluka, where development has not proceeded beyond the planning stage. Before mining commenced, a wide-ranging inquiry was held (Fox et al. 1977) and its recommendations were used as the basis for the Ranger development. One of the recommendations of the inquiry was that "a comprehensive meteorological - hydrological - water quality model of the Magela system be developed progressively as information becomes available ... (for) interpreting monitoring data ... predicting effects ... (and) planning waste water releases" (p.295). The work described in this thesis is a contribution to the Magela Creek model on the subject of the role of the aquatic plants in radionuclide flow through the floodplain. Dense stands of aquatic plants grow on the floodplain during the annual wet season and throughout much of the dry season (Williams 1979). Wetlands accumulate a variety of trace elements (Dunbabin 1983) and preliminary work on the Magela system suggested 1-1 Ficyure 1.1 Location map of Magela Creek and the - floodplains flankina the East Alligator River. Stream gauaing stations are marked GS821009 and GS821019. Vegetation Types 1. Mixed herbfield 2. Grassland 3. Undulating annual swamp and grassland 4. F o r e s t 5. Annual swamp 6. Perennial swamp J a b i l u k a Mudginberri Figure 1.2 Vegetation map of the Magela floodplain (from Williams 1979). that radium, a uranium daughter product, may be naturally accumulating at the beginning of the Magela floodplain (see Chapter 2 and Appendix A.2 based on Williams 1983a). The central hypothesis of this thesis is that effluent Ra from the Ranger mine will behave like the natural Ra and be accumulated at the beginning of the floodplain; this is called the "accumulation hypothesis". 1.3 The Buffalo-Grazing Food-Chain Asian water buffalo Bubalus bubalis graze on the floodplain and provide meat to local Aboriginals, thus making one of several potential food-chain links between any mining effluent and man (McLaughlin 1982, Koperski and Bywater 1985, Johnston in press). The International Commission on Radiological Protection (ICRP) recommends that effluent from nuclear installations be traced through the food-chain to man using mathematical models (ICRP 1979) so that the well developed standards for man can be applied to the protection of the environment as well (ICRP 1976). The buffalo-grazing food-chain is a minor one compared with the total radiological impact of the uranium mining on man; freshwater mussels, fish and dust are the major contributors (Koperski and Bywater 1985, Johnston in press). The plants have the potential to tie up a major portion of the mass of the effluent, however, and the herbivore food-chain is a convenient means of assessing its radiological significance. The mining company has been maintaining a high standard of environmental impact control and no significant radioactive pollution of the aquatic food-chain has yet been detected (OSS 1985a, Koperski 1986). The fate of radioactive effluent in the floodplain thus remains unknown and is a suitable subject for study by computational experiments on a computer simulation model. 1.4 Radioactive Wastes from Uranium Mining Uranium is the parent of 30 radioactive decay products. When uranium ore is processed for uranium extraction, most of the daughter radionuclides are left behind in the liquid, solid and gaseous wastes. The nuclides involved in the most important decay chain are listed in order of appearance in Table 1.1 together with their respective half-lives. Of the 00 f\ waste nuclides above radium-226 ( “ Ra) in the decay chain only thorium-230 has any long term relevance; it poses a significant health risk if inhaled in dust but it is chemically immobile in the aqueous environment so it is of little significance in the food 1-2 Table 1.1 The uranium-238 decay series in their order of formation. Nuclide Half-life uranium-238 4.5xl09 y thorium-234 24 d protactinium-234 6.7 h uranium-234 267000 y thorium-230 80000y radium-226 1600 y radon-222 3.8 d polonium-218 3 m actinium-2,18 2 s radon-218 0.02 s lead-214 27 s bismuth-214 20 m polonium-21| 0.2 ms thallium-210 1.3 m lead-210 22 y bismuth-210 4.9 d polonium-210 138 d thallium-206 4.2 m lead-206 stable * = yields of these nuclides are negligible. chain. Of the elements below Ra in the decay chain, those between Ra and lead-210 are too short-lived to pose any hazard in the aquadc food-chain although they may be an inhalation hazard if released to the atmosphere through escape of the noble gas radon- 222. Radium-226, lead-210 and polonium-210 are likely to be more significant than any others because they have half-lives long enough to remain active during transport and biological uptake, and they are chemically mobile in the aquatic environment. Only Ra was considered in this work because it was historically identified as the major hazard 1-3 (Tsivoglou et al. 1958, Williams and Kirchmann in press, see Appendix A.l) and more information was available on its natural background concentration in the Magela system than was the case for the other nuclides. 1.5 How Much Radium is Hazardous? While no significant pollution of the aquatic food chain has yet been detected, the potential impact of such pollution may be great. During the Ranger Uranium Environmental Inquiry (Fox et al. 1977) the evidence suggested that a doubling of the natural load of “ Ra in Magela Creek would be the maximum that the system could accept without exceeding the radiation dose limits for members of the public living off food from this source. A lot more research has been carried out since then but the data used in the most recent assessment (Johnston in press) yields a similar conclusion. The natural concentration of Ra in Magela Creek at Ranger is about 5 mBq L ' (Johnston in press) but the water monitoring that has been carried out over the years of operation at Ranger has used a limit of determination of 19 mBq L ' (Water Division 1984). Thus it is possible that almost a four-fold increase of the natural load has occurred but has not been detected. We are thus in the position that if Ra pollution is detected it will already have exceeded the statutary limit. This reasoning depends heavily on the assumption in the calculations that an increase in the Ra concentration in water will produce a linear increase in the dose to man. This will hereafter be called the "linearity hypothesis” and testing this hypothesis on the simulation model (for the buffalo-grazing food-chain) is a secondary purpose of the present work. 1.6 Literature on Radium Uptake by Aquatic Plants and Sediments The literature on radium uptake by aquatic plants is scant, consisting mainly of reports of field collections, and has been reviewed by Williams (1982) and Williams (1984a). The average concentration factor from water (CF=Ra concentration in fresh plant/Ra concentration in water) for macrophytes was 55 and the range was 2 to 20,000. There was no evidence of the sediment contributing any more Ra to the foliage than could be accounted for from the water alone. Only one experiment with vascular hydrophytes has been reported (Iskra et al. 1970); this did not include any kinetic analysis but mentioned that equilibrium was achieved within 12-15 days. Kinetic theory has never been applied in this area. In a recent review of radioecology, Coughtrey and Thome (1983) reported 1-4 that "there does not appear to have been any attempt to construct dynamic models for radionuclide accumulation and retention by aquatic plants... (nor) any general reviews' of the subject. I have therefore produced such a general review for radium and a copy is attached at Appendix A.4 (Williams in press a). More experimental work has been done on Ra uptake into sediments and into purified sediment constituents and this work has been recently reviewed by Benes (in press). Ra uptake into well mixed sediment is very rapid and equilibrates in less than 1 day and reaches distribution coefficient (A'ti=Ra concentration in dry sediment/Ra concentration in water) values ranging from 100 to 400,000 depending on the nature of the sediment and the salinity of the water.
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