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Particle-solution behaviour of plutonium in an estuarine environment, Esk Estuary, UK

Conference · · Geochimica et Cosmochimica Acta; (United States)
OSTI ID:5852966
; ;  [1];  [2]
  1. Lancaster Univ. (United Kingdom)
  2. Plymouth Marine Laboratory, West Hoe (United Kingdom)
The particle-solution (K[sub d]) relationships of Pu(III,IV) in the Esk Estuary are investigated, using new experimental data together with a synthesis of earlier work. Adsorption of [sup 236]Pu(IV) by a suspension of intertidal mud (40 mg L[sup [minus]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 [sup 239,240]Pu(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 [sup 239,240]Pu(II,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) K[sub d] on sediment concentration. Thus, a single K[sub d] 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 [sup 239,240]Pu(III,IV) fraction. For example, in R. Esk water, the adsorption of [sup 236]Pu(III,IV) and the desorption of [sup 239,240]Pu(III,IV), over a two order of magnitude concentration range of unwashed Esk Estuary sediment, can be accounted for by a single K[sub d] of [approximately]3 [times] 10[sup 3] L kg[sup [minus]1]. The K[sub d] 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[sup +] 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.
OSTI ID:
5852966
Report Number(s):
CONF-911017--; CNN: PECD 7/9/429
Conference Information:
Journal Name: Geochimica et Cosmochimica Acta; (United States) Journal Volume: 57:14
Country of Publication:
United States
Language:
English