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Anaerobic Biotransformation and Mobility of Pu and of Pu-EDTA

Description: The enhanced mobility of radionuclides by co-disposed chelating agent, ethylenediaminetetraacetate (EDTA), is likely to occur only under anaerobic conditions. Our extensive effort to enrich and isolate anaerobic EDTA-degrading bacteria has failed. Others has tried and also failed. To explain the lack of anaerobic biodegradation of EDTA, we proposed that EDTA has to be transported into the cells for metabolism. A failure of uptake may contribute to the lack of EDTA degradation under anaerobic conditions. We demonstrated that an aerobic EDTA-degrading bacterium strain BNC1 uses an ABC-type transporter system to uptake EDTA. The system has a periplasmic binding protein that bind EDTA and then interacts with membrane proteins to transport EDTA into the cell at the expense of ATP. The bind protein EppA binds only free EDTA with a Kd of 25 nM. The low Kd value indicates high affinity. However, the Kd value of Ni-EDTA is 2.4 x 10^(-10) nM, indicating much stronger stability. Since Ni and other trace metals are essential for anaerobic respiration, we conclude that the added EDTA sequestrates all trace metals and making anaerobic respiration impossible. Thus, the data explain the lack of anaerobic enrichment cultures for EDTA degradation. Although we did not obtain an EDTA degrading culture under anaerobic conditions, our finding may promote the use of certain metals that forms more stable metal-EDTA complexes than Pu(III)-EDTA to prevent the enhanced mobility. Further, our data explain why EDTA is the most dominant organic pollutant in surface waters, due to the lack of degradation of certain metal-EDTA complexes.
Date: November 20, 2009
Creator: Xun, Luying
Partner: UNT Libraries Government Documents Department

Field-Portable Immunoassay Instruments and Reagents to Measure Chelators and Mobile Forms of Uranium

Description: Previous studies from our laboratory have demonstrated the feasibility of immunoassays for identification and quantification of specific metal ions. Our ultimate goal for this project is to (1) isolate and characterize antibodies that recognize the most mobile form of uranium, UO22+; (2) assemble, test, and validate a new field-portable immunosensor based on these antibodies; (3) prepare new monoclonal antibodies to the primary chelators (EDTA and DTPA) found in DOE wastes.
Date: June 1, 2001
Creator: Blake, Diane A.
Partner: UNT Libraries Government Documents Department


Description: BS>The separation of rare earth mixtures by ion exchange using ammonium ethylenedisminetetracetate and annmonium N-hydroxyethylethylenediaminetriacetate as eluting agents is discussed in detail. Simple countercurrent separation theory is used to predict the minimum nuinber of displacements of an adsorbed band that are necessary in order to separate the components of binary mixtures. It is shown how the theory can be applied to even more complex systems, and experimental data are presented for some of the more difficultly separablc groups of rare-earth species. Experimental results agree very well with the theoretical predictions. (auth) A detailed description is presented of a process developed by Ames Laboratory for the separation of thorium, rare earths, and uranium from monazite sands. Oxalic acid is used to precipitate rare earths; and thorium from a sulfate and phosphate solution of these elements. The possibility of recovering uranium from the oxalate filtrate by anion exchange was investigated. (W.L.H.)
Date: January 1, 1956
Creator: Powell, J.E. & Spedding, F.H.
Partner: UNT Libraries Government Documents Department

Biotransformation of PuEDTA: Implications to Pu Immobilization

Description: This project integrates three distinct goals to develop a fundamental understanding of the potential fate and disposition of plutonium in sediments that are co-contaminated with EDTA. The three objectives are: (1) Develop thermodynamic data for Pu-EDTA species and determine the dominant mobile form of Pu under anaerobic conditions. (2) Elucidate the mechanism and rates of Pu(IV) and Pu(IV)-EDTA reduction by metal-reducing bacteria and determine where the Pu is located (in solution, biosorbed, bioaccumulated). (3) Enrich and isolate anaerobic EDTA-degrading microorganisms to investigate the anaerobic biodegradation of Pu-EDTA.
Date: June 1, 2006
Creator: Bolton, Harvey, Jr.
Partner: UNT Libraries Government Documents Department

Outer Sphere Adsorption of Pb(II)EDTA on Goethite

Description: FTIR and EXAFS spectroscopic measurements were performed on Pb(II)EDTA adsorbed on goethite as functions of pH (4-6), Pb(II)EDTA concentration (0.11 {micro}M - 72 {micro}M), and ionic strength (16 {micro}M - 0.5M). FTIR measurements show no evidence for carboxylate-Fe(III) bonding or protonation of EDTA at Pb:EDTA = 1:1. Both FTIR and EXAFS measurements suggest that EDTA acts as a hexadentate ligand, with all four of its carboxylate and both amine groups bonded to Pb(II). No evidence was observed for inner-sphere Pb(II)-goethite bonding at Pb:EDTA = 1:1. Hence, the adsorbed complexes should have composition Pb(II)EDTA{sup 2{minus}}. Since substantial uptake of PbEDTA(II){sup 2{minus}} occurred in the samples, we infer that Pb(II)EDTA{sup 2{minus}} adsorbed as outer-sphere complexes and/or as complexes that lose part of their solvation shells and hydrogen bond directly to goethite surface sites. We propose the term ''hydration-sphere'' for the latter type of complexes because they should occupy space in the primary hydration spheres of goethite surface functional groups, and to distinguish this mode of sorption from common structural definitions of inner- and outer-sphere complexes. The similarity of Pb(II) uptake isotherms to those of other divalent metal ions complexed by EDTA suggests that they too adsorb by these mechanisms. The lack of evidence for inner-sphere EDTA-Fe(III) bonding suggests that previously proposed metal-ligand - promoted dissolution mechanisms should be modified, specifically to account for the presence of outer-sphere precursor species.
Date: July 16, 1999
Creator: Bargar, John R
Partner: UNT Libraries Government Documents Department

Low Temperature Polymeric Precursor Derived Zinc Oxide Thin Films

Description: Zinc oxide (ZnO) is a versatile environmentally benign II-VI direct wide band gap semiconductor with several technologically plausible applications such as transparent conducting oxide in flat panel and flexible displays. Hence, ZnO thin films have to be processed below the glass transition temperatures of polymeric substrates used in flexible displays. ZnO thin films were synthesized via aqueous polymeric precursor process by different metallic salt routes using ethylene glycol, glycerol, citric acid, and ethylene diamine tetraacetic acid (EDTA) as chelating agents. ZnO thin films, derived from ethylene glycol based polymeric precursor, exhibit flower-like morphology whereas thin films derived of other precursors illustrate crack free nanocrystalline films. ZnO thin films on sapphire substrates show an increase in preferential orientation along the (002) plane with increase in annealing temperature. The polymeric precursors have also been used in fabricating maskless patterned ZnO thin films in a single step using the commercial Maskless Mesoscale Materials Deposition system.
Date: December 2006
Creator: Choppali, Uma
Partner: UNT Libraries

Anaerobic Biotransformation and Mobility of Pu and PuEDTA

Description: The objective of this report is to isolate anaerobic EDTA-degrading bacteria. Although our goal is to isolate anaerobic EDTA degraders, we initiated the experiments to include nitrilotriacetate (NTA), which is a structure homologue of EDTA. All the aerobic EDTA degraders can degrade NTA, but the isolated NTA degraders cannot degrade EDTA. Since NTA is a simpler structure homologue, it is likely that EDTA-degrading ability is evolved from NTA degradation. This hypothesis is further supported from our characterization of EDTA and NTA-degrading enzymes and genes (J. Bact. 179:1112-1116; and Appl. Environ. Microbiol. 67:688-695). The EDTA monooxygenase and NTA monooxygenase are highly homologous. EDTA monooxygenase can use both EDTA and NTA as substrates, but NTA monooxygenase can only use NTA as a substrate. Thus, we put our effort to isolate both NTA and EDTA degraders. In case, an anaerobic EDTA degrader is not immediately enriched, we will try to evolve the NTA degraders to use EDTA. Both aerobic and anaerobic enrichment cultures were set.
Date: June 1, 2005
Creator: Xun, Luying
Partner: UNT Libraries Government Documents Department

Biodegradation of PuEDTA and Impacts on Pu Mobility

Description: This project is part of a major project (PI, Dr. Harvey Bolton, Jr. at PNNL) regarding plutonium mobility in the subsurface. Ethylenediaminetetraacetate (EDTA) is a common chelating agent that can increase the mobility of radionuclides and heavy metals in groundwater. Biodegradation of EDTA decreases the enhanced mobility. The overall objective is to understand how microbial degradation affects Plutonium-EDTA transport in the environment, and the specific objective of this component is to understand how microorganisms degrade EDTA. Over the past two years, significant progress has been made to the understanding on how EDTA is degraded by an EDTA-degrading bacterium BNC1. The characterization of EDTA and nitrilotriacetate (NTA) transport into BNC1 cells is summarized here. The uptake is the limiting step in EDTA and NTA degradation. The objectives of near-term research are described. We are making progress as projected in the proposal.
Date: June 1, 2003
Creator: Xun, Luying & Bolton, Harvey, Jr.
Partner: UNT Libraries Government Documents Department

Chemical Characterization of Soluble Phosphorus Forms along a Hydrologic Flowpath of a Forested Stream Ecosystem

Description: The concentration and distribution of soluble phosphorus (P) forms were determined in compartments of a hydrologic pathway in a forested watershed (Walker Branch, Tennessee). Rainfall, throughfall, soil water, groundwater, stream water, and water from two sites in Melton Hill reservoir downstream of Walker Branch were examined for soluble reactive and total soluble phosphorus (SRP and TSP). Soluble unreactive P (SUP) was determined from their difference. An increase of TSP from rainfall to throughfall indicated leaching or wash off of P from the canopy. SRP and SUP decreased markedly as water percolated through the soil, suggesting biological uptake and/or geochemical adsorption of phosphate groups on soil particles. Changes in soluble P. concentrations within the stream channel supported previous evidence for biological control of P dynamics in Walker Branch. Overall, SUP (an estimate of soluble organic P) constituted a significant fraction of the total soluble P present in each compartment of the flowpath. An analytical technique using high-performance liquid chromatography (HPLC) to separate the inositol phosphates (IP's) was developed and used in characterizing organic P fractions of natural systems. Commercial orthophosphate, inositol monophosphate (IMP), and inositol hexaphosphate (IHP) were adequately separated from each other on Aminex A-27 resin using a sodium chloride/tetrasodium EDTA gradient elution. The technique was used to separate an enzyme hydrolysate mixture of IP's into five components. IHP was separated from PO{sub 4} and IMP in a wheat bran extract using the HPLC method. Alkaline bromination was used to extract IP's from a Walker Branch soil sample and HPLC was used to examine the extract; at least three IP peaks were recognized. Using the HPLC technique, an attempt was made to detect the presence of IP's in a Walker Branch groundwater sample concentration by ultrafiltration. The concentration process was unsuccessful possibly due to filtration membrane leakage, so no peaks ...
Date: January 1, 1999
Creator: Segars, J.E.
Partner: UNT Libraries Government Documents Department

Photo-oxidation of organic compounds in liquid low-level mixed wastes at the INEL

Description: A bench-scale oxidation apparatus is implemented to study the effectiveness of using an artificial ultraviolet source, a 175-watt medium pressure mercury vapor lamp, to enhance the destruction of organic contaminants in water with chemical oxidants. The waste streams used in this study are samples or surrogates of mixed wastes at the Idaho National Engineering Laboratory. The contaminants that are investigated include methylene chloride, 1,1,1-trichlorethane, 1, 1-dichlororethane, acetone, 2-propanol, and ethylenediamine tetraacetic acid. We focus on H{sub 2}O{sub 2}-based oxidizers for our treatment scheme, which include the UV/H{sub 2}O{sub 2} system, the dark Fenton system (H{sub 2}O{sub 2}/Fe{sup 2+}), and the photo- assisted Fenton system (UV/H{sub 2}O{sub 2}/Fe{sup 3+}) is used in particular. Variables include concentration of the chemical oxidizer, concentration of the organic contaminant, and the elapsed reaction time. Results indicate that the photo-assisted Fenton system provides the best overall performance of the oxidizing systems listed above, where decreases in concentrations of methylene chloride, 1,1,1- trichloroethane, 1,1-dichlororethane, 2-propanol, and ethylenediamine tetraacetic acid were seen. However, UV-oxidation treatment provided no measurable benefit for a mixed waste containing acetone in the presence of 2-propanol.
Date: August 1, 1996
Creator: Gering, K.L. & Schwendiman, G.L.
Partner: UNT Libraries Government Documents Department

Equilibrium characteristics of tartrate and EDTA-based electroless copper deposition baths

Description: Electroless deposition of copper is being used for a variety of applications, one of them being the development of seed metallic layers on non-metals, which are widely used in electronic circuitry. Solution equilibrium characteristics of two electroless copper baths containing EDTA and tartrate as the complexing agents were studied as functions of pH, chelating agent and metal ion concentrations. Equilibrium diagrams were constructed for both cu-tartrate and Cu-EDTA systems. It was determined that copper is chiefly complexed as Cu(OH){sub 2}L{sub 2}{sup {minus}4} in the tartrate bath, and as CuA{sup {minus}2} in the EDTA bath, where L and A are the complexing tartrate and EDTA ligands, respectively. The operating ranges for electroless copper deposition were identified for both baths. Dependence of Cu(OH){sub 2} precipitation on the pH and species concentrations was also studied for these systems.
Date: August 1, 1997
Creator: Ramasubramanian, M.; Popov, B.N.; White, R.E. & Chen, K.S.
Partner: UNT Libraries Government Documents Department

Sorption and diffusion studies of Pu(IV) and Pu(V)-EDTA onto and through Hanford soil

Description: Plutonium production at U.S. Department of Energy Hanford site has created massive amounts of radioactive and mixed wastes. Over 1.3 trillion liters of liquid waste have been discharged into the ground, the largest part of which has been absorbed by the upper soil layers with a small fraction migrating into the groundwater. Approximately 350 million liters of other low and high-level mixed wastes were stored in underground tanks between 1944 and 1980. These tanks contain organic materials that were introduced during the production and processing of plutonium, such as ethylenediametetraacetic acid (EDTA), tributyl phosphate, hexone, paraffin hydrocarbon and other minor organic and inorganic components. The quantity of EDTA is estimated to be 83 metric tons in the underground tanks. Several single-shell tanks are known or suspected to have leaked. It was reported that since 1995, approximately four million liters of mixed waste might have entered the soil beneath the single-shell tanks. This volume of waste is estimated to contain as much as one million curies of radioactivity.
Date: September 15, 1999
Creator: Allen, P G; Hakem, N L & Sylwester, E R
Partner: UNT Libraries Government Documents Department

Radionuclide-Chelating Agent Complexes in Low-Level Radioactive Decontamination Waste; Stability, Adsorption and Transport Potential

Description: Speciation calculations were done to determine whether organic complexants facilitate transport of radionuclides leached from waste buried in soils. EDTA readily mobilizes divalent transition metals and moderately impacts trivalent actinides. Picolinate readily mobilizes only Ni2+ and Co2+. These speciation predictions ignore the influence of soil adsorption and biodegradation that break apart the complexes. In adsorption studies, picolinate concentrations have to be >10-4 M to lower the adsorption of Ni and Co. For Sm(III), Th(IV), Np(V), U(VI), and Pu, the picolinate concentration must be >10-3 M before adsorption decreases. EDTA forms strong complexes with divalent transition metals and can stop adsorption of Ni and Co when EDTA solution concentrations are 10-5 M. EDTA complexes with Np(V), U(VI), and Pu are much weaker; EDTA concentrations would have to be >10-3 M to adversely effects non-transition metal/radionuclide adsorption. Most picolinate and ETDA-metal complexes appear to readily dissociate during interactions with soils. The enhanced migration of radionuclide-organic complexes may be limited to a few unique conditions. We recommend that mixtures of metal/radionuclides and EDTA should not be solidified or co-disposed with high pH materials such as cement. For weaker binding organic complexants, such as picolinate, citrate and oxalate, co-disposal of decontamination wastes and concrete should be acceptable.
Date: February 1, 2002
Creator: Serne, R. Jeffrey; Cantrell, Cantrell J.; Lindenmeier, Clark W.; Owen, Antionette T.; Kutnyakov, Igor V.; Orr, Robert D. et al.
Partner: UNT Libraries Government Documents Department

Thermal Stability of Chelated Indium Activable Tracers

Description: The thermal stability of indium tracer chelated with organic ligands ethylenediaminetetraacetic acid (EDTA) and nitrilotriacetic acid (NTA) was measured for reservoir temperatures of 150, 200, and 240 C. Measurements of the soluble indium concentration was made as a function of time by neutron activation analysis. From the data, approximate thermal decomposition rates were estimated. At 150 C, both chelated tracers were stable over the experimental period of 20 days. At 200 C, the InEDTA concentration remained constant for 16 days, after which the thermal decomposition occurred at a measured rate constant of k = 0.09 d{sup -1}. The thermal decomposition of InNTA at 200 C showed a first order reaction with a measured rate constant of k = 0.16 d{sup -1}. At 240 C, both indium chelated tracers showed rapid decomposition with rate constants greater than 1.8 d{sup -1}. The data indicate that for geothermal reservoir with temperatures up to about 200 C, indium chelated tracers can be used effectively for transit times of at least 20 days. These experiments were run without reservoir rock media, and do not account for concomitant loss of indium tracer by adsorption processes.
Date: January 21, 1986
Creator: Chrysikopoulos, Costas & Kruger, Paul
Partner: UNT Libraries Government Documents Department

Biodegradation of PuEDTA and Impacts on Pu Mobility

Description: Ethylenediaminetetraacetate (EDTA) and nitrilotriacetate (NTA) are synthetic chelating agents, which can form strong water-soluble complexes with radionuclides and metals and has been used to decontaminate and process nuclear materials. Synthetic chelating agents were co-disposed with radionuclides (e.g., 60Co, Pu) and heavy metals enhancing their transport in the subsurface. An understanding of EDTA biodegradation is essential to help mitigate enhanced radionuclide transport by EDTA. The objective of this research is to develop fundamental data on factors that govern the biodegradation of radionuclide-EDTA. These factors include the dominant EDTA aqueous species, the biodegradation of various metal-EDTA complexes, the uptake of various metal-EDTA complexes into the cell, the distribution and mobility of the radionuclide during and after EDTA biodegradation, and the enzymology and genetics of EDTA biodegradation.
Date: June 1, 2001
Creator: Xun, Luying & Bolton, Jr., Harvey
Partner: UNT Libraries Government Documents Department

Biodegradation of PuEDTA and Impacts on Pu Mobility

Description: This project, by Dr. Xun, supports work at PNNL (Bolton) regarding plutonium mobility in the subsurface. Ethylenediaminetetraacetate (EDTA) is a chelating agent that can increase the mobility of radionuclides and heavy metals in groundwater. Biodegradation of EDTA can decrease the enhanced mobility. The overall objective is to understand how microbial degradation affects Plutonium-EDTA transport in the environment and the specific objective of this component is to understand how microorganisms degrade EDTA. A chelating degrading bacterium BNC1 can use EDTA and nitrilotriacetate (NTA) as sole carbon and nitrogen sources. A gene cluster responsible for both EDTA and NTA degradation has been cloned and characterized (1,2). The same enzymes are used to degrade both compounds except that additional enzymes are required for EDTA degradation. Since the enzymes are located inside cells, EDTA and NTA must be transported into cells for degradation. For the first funding year, we have focused on how EDTA and NTA are transported into BNC1 cells. The EDTA-degrading gene cluster also contains genes encoding a hypothetical ABC-type transporter. We first demonstrated that the transporter genes and EDTA monooxygenase gene (emoA) were co-transcribed by RT-PCR, suggesting that the genes are involved in EDTA transport. We then characterized one of the gene product EppA. Using recombinant EppA purified from Escherichia coli, we have shown that EppA binds several metal:EDTA complexes by fluorescence techniques. In addition, EppA is shown to bind Mg:NTA, Ca:NTA and Fe(III):NTA but not free NTA.
Date: June 1, 2002
Creator: Xun, Luying & Bolton, Jr., Harvey
Partner: UNT Libraries Government Documents Department