Nonreversible Immobilization of Water-Borne Plutonium onto Self-Assembled Adlayers of Silanized Humic Materials

摘要

The objective was to study plutonium parti- tioning between immobile and mobile humic materials at the water-solid interfaces. Immobilization of the humic materials on solid supports was performed in situ using self-adhesive silanized humic derivatives. The presence of the humic adlayers on solid supports was shown to significantly enhance Pu sorption and its retention under both steady state and dynamic conditions. While plutonium may exist in multiple oxidations states plus colloidal forms, the major thrust in this work was to study the behavior of most mobile - the PuO_2~+ form in dilute solutions. The values of the plutonium partition coefficients (K_d) between water and humics-coated silica gels after 10 days exposure reached 1.6 × 10~4 L·kg~(-1) at pH 7.5 under anaerobic conditions with a total plutonium concentration of 1.2 × 10~(-8) M exceeding those for the uncoated SiO_2 (6.3 × 10~2 L·kg~(-1)). Column tests showed substantial sequestration of water-borne plutonium (up to 73%) on the humics-coated silica gels. Remobilization experiments conducted under batch conditions at different pH values (3.5, 4.5, 7.5) showed that no more than 3% of the sequestered Pu was remobilized from the humics-coated silica gels by treatment with dissolved humic materials at environmentally relevant pH of 7.5. Consequently, silanized humic materialas can be seen as both molecular probes and as potent candidate materials for scavenging mobile Pu from an aqueous phase.