Particle-solution behaviour of plutonium in an estuarine environment,Esk Estuary,UK |
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| Institution: | 1. South China Sea Environment Monitoring Center, State Oceanic Administration (SOA), Guangzhou 510300, Guangdong, PR China;2. South China Sea Testing and Appraisal Center, State Oceanic Administration (SOA), Guangzhou 510300, Guangdong, PR China;3. Guangdong Institute of Analysis, Guangdong Provincial Key Laboratory of Emergency Test for Dangerous Chemicals, Guangzhou 510070, Guangdong, PR China;1. South China Sea Fisheries Research Institute, Chinese Academy of Fishery Sciences, Guangzhou 510300, China;2. Key Laboratory of Fishery Ecology and Environment of Guangdong Province, Guangzhou 510300, China;3. Key Laboratory of Ministry of Agriculture for South China Sea Fishery Resources Exploitation & Utilization, Guangzhou 510300, China;4. State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China;5. Center of Fishery Resources and Ecology Environment Research, Chinese Academy of Fishery Sciences, Beijing 100141, China |
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| Abstract: | The particle-solution (Kd) relationships of Pu(III,IV) in the Esk Estuary are investigated, using new experimental data together with a synthesis of our earlier work. Adsorption of 236Pu(IV) by a suspension of intertidal mud (40 mg L?1) from the Esk Estuary was determined after 1 h, as a function of salinity and pH, in a series of controlled laboratory experiments. Desorption of 239, 240Pu(III,IV) from this environmentally contaminated sediment was determined concurrently. The short term (i.e., within a tidal cycle) non-conservative behaviour of Pu(III,IV) in both the laboratory experiments and the estuary appears to be dominated by a rapid, reversible surface complexation reaction, although only a small fraction (<5%) of the 239,240Pu(III,IV) activity of the environmentally contaminated sediment is able to participate in the reaction. The existence of this exchangeable or labile fraction can explain the apparent dependence of Pu(III,IV) Kd on sediment concentration. Thus, a single Kd value is able to describe both the observed adsorption and desorption behaviour and the effect of sediment concentration, when desorption is expressed with respect to the labile 239,240Pu(III,IV) fraction. For example, in R. Esk water, the adsorption of 236Pu(III,IV) and the desorption of 236,240Pu(III,IV), over a two order of magnitude concentration range of unwashed Esk Estuary sediment, can be accounted for by a single Kd of ～3 × 103 L kg?1. The Kd for the labile Pu(III,IV) fraction varies mainly as a function of salinity. pH is not an important factor over the pH range 4–9, although H+ ion exchange does occur, probably through a similar surface complexation reaction. The kinetic and equilibrium characteristics of the Pu (III,IV) sorption behaviour conform to the pattern observed by Jannasch et al. (1988) and other workers for a range of trace elements. |
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