Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA

Conference · Wed Apr 05 00:00:00 EDT 2006

OSTI ID:894572

Bailey, V L; Plymale, A E; Rai, D; Xun, L

The complexation of radionuclides (e.g., plutonium (Pu) and {sup 60}Co) by co-disposed ethylenediaminetetraacetate (EDTA) has enhanced their transport in sediments at DOE sites. Pu(IV)-EDTA is not stable in the presence of relatively soluble Fe(III) compounds. Since most DOE sites have Fe(III) containing sediments, Pu(IV) is likely not the mobile form of Pu-EDTA. The only other Pu-EDTA complex stable in groundwater relevant to DOE sites would be Pu(III)-EDTA, which only forms under anaerobic conditions. Research is therefore needed to investigate the biotransformation of Pu and Pu-EDTA under anaerobic conditions and the anaerobic biodegradation of Pu-EDTA. The biotransformation of Pu and Pu-EDTA under various anaerobic regimes is poorly understood including the reduction kinetics of Pu(IV) to Pu(III) from soluble (Pu(IV)-EDTA) and insoluble Pu(IV), the redox conditions required for this reduction, the strength of the Pu(III)-EDTA, how the Pu(III)-EDTA competes with other dominant anoxic soluble metals (e.g., Fe(II)), and the oxidation kinetics of Pu(III)-EDTA. Finally, soluble Pu(III)-EDTA under anaerobic conditions would require anaerobic degradation of the EDTA to limit Pu(III) transport. Anaerobic EDTA degrading microorganisms have never been isolated. Recent results have shown that Shewanella oneidensis MR-1, a dissimilatory metal reducing bacterium, can reduce Pu(IV) to Pu(III). The Pu(IV) was provided as insoluble PuO2. The highest rate of Pu(IV) reduction was with the addition of AQDS, an electron shuttle. Of the total amount of Pu solubilized (i.e., soluble through a 0.36 nm filter), approximately 70% was Pu(III). The amount of soluble Pu was between 4.8 and 3.2 micromolar at day 1 and 6, respectively, indicating rapid reduction. The micromolar Pu is significant since the drinking water limit for Pu is 10{sup -12} M. On-going experiments are investigating the influence of EDTA on the rate of Pu reduction and the stability of the formed Pu(III). We have also begun to enrich and isolate bacteria capable of aerobic and anaerobic degradation of EDTA. Environmental samples (e.g., sludges, river sediments) were incubated aerobically and anaerobically with EDTA or NTA as the sole carbon and energy source. Aerobic enrichment with EDTA has not resulted in any cultures, but NTA has provided several isolates. Partial 16S rRNA gene sequence and sequence comparison identified four separate strains closely related to Microbacterium oxydans, Aminobacter sp., Achromobacter sp., Aminobacter sp., respectively. Anaerobic enrichments with either EDTA or NTA are still in progress since metabolism and growth is relatively slow. In addition to the biotransformation experiments, studies are underway to determine/validate complexation constants of Pu(III) with EDTA and the influence of competing ions on Pu(III)-EDTA complexes. These data are being obtained through solubility studies of PuPO{sub 4}(s) and Pu(OH){sub 3}(s) as a function of time, pH, and EDTA and competing ion concentrations. These results have begun to fill-in knowledge gaps of how anaerobic conditions will influence Pu and Pu-EDTA fate and transport to assess, model, and design approaches to stop Pu transport in groundwater at DOE sites.

• Research Organization: Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State University, Pullman, WA
• Sponsoring Organization: USDOE Office of Science (SC)
• OSTI ID: 894572
• Report Number(s): CONF-ERSP2006-34; TRN: US0700186
• Resource Relation: Conference: Annual Environmental Remediation Sciences Program PI Meeting, April 3-5, 2006, Warrenton, VA
• Country of Publication: United States
• Language: English

Related Subjects

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
54 ENVIRONMENTAL SCIENCES
59 BASIC BIOLOGICAL SCIENCES
ANAEROBIC CONDITIONS
BACTERIA
BIODEGRADATION
CARBON
DRINKING WATER
EDTA
ELECTRONS
ENERGY SOURCES
GENES
KINETICS
METABOLISM
MICROORGANISMS
OXIDATION
PLUTONIUM
RADIOISOTOPES
SEDIMENTS
SLUDGES
SOLUBILITY