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Title: Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA

Abstract

The complexation of radionuclides (e.g., plutonium (Pu) and {sup 60}Co) by codisposed ethylenediaminetetraacetate (EDTA) has enhanced their transport in sediments at DOE sites. Our previous NABIR research investigated the aerobic biodegradation and biogeochemistry of Pu(IV)-EDTA. Plutonium(IV) forms stable complexes with EDTA under aerobic conditions and an aerobic EDTA degrading bacterium can degrade EDTA in the presence of Pu and decrease Pu mobility. However, our recent studies indicate that while Pu(IV)-EDTA is stable in simple aqueous systems, it is not stable in the presence of relatively soluble Fe(III) compounds (i.e., Fe(OH){sub 3}(s)--2-line ferrihydrite). Since most DOE sites have Fe(III) containing sediments, Pu(IV) in likely not the mobile form of Pu-EDTA in groundwater. 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 in this brand new project to investigate the biotransformation of Pu and Pu-EDTA under anaerobic conditions. 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) as PuO2(am) by metal reducing bacteria, the redox conditions required for this reduction, the strength of the Pu(III)-EDTA complex, how themore » Pu(III)-EDTA complex competes with other dominant anoxic soluble metals (e.g., Fe(II)), and the oxidation kinetics of Pu(III)-EDTA. Finally, the formation of a stable soluble Pu(III)-EDTA complex under anaerobic conditions would require degradation of the EDTA complex to limit Pu(III) transport in geologic environments. Anaerobic EDTA degrading microorganisms have not been isolated. These knowledge gaps preclude the development of a mechanistic understanding 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.« less

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA; Washington State University, Pullman, WA
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
895005
Report Number(s):
CONF-NABIR2005-8
TRN: US0700367
Resource Type:
Conference
Resource Relation:
Conference: Annual NABIR PI Meeting, April 18, 2005, Warrenton, VA
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; 59 BASIC BIOLOGICAL SCIENCES; AEROBIC CONDITIONS; ANAEROBIC CONDITIONS; BACTERIA; BIODEGRADATION; BIOGEOCHEMISTRY; DESIGN; EDTA; KINETICS; MICROORGANISMS; OXIDATION; PLUTONIUM; RADIOISOTOPES; SEDIMENTS

Citation Formats

Bolton, H., Jr., Rai, D., and Xun, L. Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA. United States: N. p., 2005. Web.
Bolton, H., Jr., Rai, D., & Xun, L. Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA. United States.
Bolton, H., Jr., Rai, D., and Xun, L. Mon . "Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA". United States. https://www.osti.gov/servlets/purl/895005.
@article{osti_895005,
title = {Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA},
author = {Bolton, H., Jr. and Rai, D. and Xun, L.},
abstractNote = {The complexation of radionuclides (e.g., plutonium (Pu) and {sup 60}Co) by codisposed ethylenediaminetetraacetate (EDTA) has enhanced their transport in sediments at DOE sites. Our previous NABIR research investigated the aerobic biodegradation and biogeochemistry of Pu(IV)-EDTA. Plutonium(IV) forms stable complexes with EDTA under aerobic conditions and an aerobic EDTA degrading bacterium can degrade EDTA in the presence of Pu and decrease Pu mobility. However, our recent studies indicate that while Pu(IV)-EDTA is stable in simple aqueous systems, it is not stable in the presence of relatively soluble Fe(III) compounds (i.e., Fe(OH){sub 3}(s)--2-line ferrihydrite). Since most DOE sites have Fe(III) containing sediments, Pu(IV) in likely not the mobile form of Pu-EDTA in groundwater. 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 in this brand new project to investigate the biotransformation of Pu and Pu-EDTA under anaerobic conditions. 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) as PuO2(am) by metal reducing bacteria, the redox conditions required for this reduction, the strength of the Pu(III)-EDTA complex, how the Pu(III)-EDTA complex competes with other dominant anoxic soluble metals (e.g., Fe(II)), and the oxidation kinetics of Pu(III)-EDTA. Finally, the formation of a stable soluble Pu(III)-EDTA complex under anaerobic conditions would require degradation of the EDTA complex to limit Pu(III) transport in geologic environments. Anaerobic EDTA degrading microorganisms have not been isolated. These knowledge gaps preclude the development of a mechanistic understanding 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.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2005},
month = {4}
}

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