TY - JOUR

T1 - Particle-solution behaviour of plutonium in an estuarine environment, Esk Estuary, UK.

AU - Hamilton-Taylor, J.

AU - Kelly, M.

AU - Titley, J. G.

AU - Turner, D. R.

PY - 1993/7

Y1 - 1993/7

N2 - 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.

AB - 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.

U2 - 10.1016/0016-7037(93)90545-8

DO - 10.1016/0016-7037(93)90545-8

M3 - Journal article

VL - 57

SP - 3367

EP - 3381

JO - Geochimica et Cosmochimica Acta

JF - Geochimica et Cosmochimica Acta

IS - 14

ER -