Biotransformation of plutonium complexed with citric acid

Abstract

The presence of organic ligands in radioactive wastes is a major concern because of their potential for increasing the transport of radionuclides from disposal sites. Biotransformation of radionuclides complexed with organic ligands should precipitate the radionuclides and retard their migration. We investigated the biotransformation of Pu(IV) (10-8to 10-5M), byPseudomonas fluorescensin the presence of excess citric acid. Analysis of242Pu-citrate by electrospray ionization-mass spectrometry (ESI-MS) indicated the presence of biligand Pucit2as the predominant complex. XANES and EXAFS analyses showed that Pu was in the +4 oxidation state and associated with citric acid as a mononuclear complex. Citric acid was metabolized byP. fluorescensat a rate of 4.9 μM/h, but in the presence of 10-8and 10-6M Pu, this rate decreased to 4.0 and 3.8 μM/h, respectively. An increase in the ionic strength of the medium from 0.18 M to 0.9 M lowered citrate metabolism by ∼65%. Pu added to the growth medium in the absence of bacteria remained as Pu(IV) in solution as a complex with citric acid. However, solvent extraction by thenoyltrifluoroacetone (TTA) and microfiltration (0.03 μm) of the medium containing bacteria after citrate biodegradation revealed the presence of polymeric Pu. The extent of formation of the Pu polymer depended on the Pu:citrate ratio, the extent of citrate metabolism, and the ionic strength of the medium.