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THE DISCOVERY OF THE TRANSURANIUM ELEMENTS: THEIR HISTORY AND A PRESENTATION OF THE DIFFERENT METHODS USED IN THEIR DISCOVERY

Description: BS>The ten transuranium elements discovered since 1940 are discussed in chronological order. The discoverer, the history, and methods used are given for each element. Future developments in the discovery and preparation of transuranic elements are discussed. (A.C.)
Date: April 1, 1959
Creator: Thompson, S.G.
Partner: UNT Libraries Government Documents Department

The Estimation of Heats of Formation

Description: The procedure for estimation of heats of formation of compounds is illustrated by discussion of compounds of several of the elements of the actinide series. The procedure is particularly suited for lanthanide and actinide elements because of the similarity of the ionic radii and types of bonding.
Date: February 2, 1948
Creator: Brewer, Leo
Partner: UNT Libraries Government Documents Department

Complexation of Actinides in Solution: Thermodynamic Measurementsand Structural Characterization

Description: This paper presents a brief introduction of the studies of actinide complexation in solution at Lawrence Berkeley National Laboratory. An integrated approach of thermodynamic measurements and structural characterization is taken to obtain fundamental understanding of actinide complexation in solution that is of importance in predicting the behavior of actinides in separation processes and environmental transport.
Date: February 1, 2007
Creator: Rao, L.
Partner: UNT Libraries Government Documents Department

Complexation of Gluconate with Uranium(VI) in Acidic Solutions: Thermodynamic Study with Structural Analysis

Description: Within the pC{sub H} range of 2.5 to 4.2, gluconate forms three uranyl complexes UO{sub 2}(GH{sub 4}){sup +}, UO{sub 2}(GH{sub 3})(aq), and UO{sub 2}(GH{sub 3})(GH{sub 4}){sup -}, through the following reactions: (1) UO{sub 2}{sup 2+} + GH{sub 4}{sup -} = UO{sub 2}(GH{sub 4}){sup +}, (2) UO{sub 2}{sup 2+} + GH{sub 4}{sup -} = UO{sub 2}(GH{sub 3})(aq) + H{sup +}, and (3) UO{sub 2}{sup 2+} + 2GH{sub 4}{sup -} = UO{sub 2}(GH{sub 3})(GH{sub 4}){sup -} + H{sup +}. Complexes were inferred from potentiometric, calorimetric, NMR, and EXAFS studies. Correspondingly, the stability constants and enthalpies were determined to be log {Beta}{sub 1} = 2.2 {+-} 0.3 and {Delta}H{sub 1} = 7.5 {+-} 1.3 kJ mol{sup -1} for reaction (1), log {Beta}{sub 2} = -(0.38 {+-} 0.05) and {Delta}H{sub 2} = 15.4 {+-} 0.3 kJ mol{sup -1} for reaction (2), and log {Beta}{sub 3} = 1.3 {+-} 0.2 and {Delta}H{sub 3} = 14.6 {+-} 0.3 kJ mol{sup -1} for reaction (3), at I = 1.0 M NaClO{sub 4} and t = 25 C. The UO{sub 2}(GH{sub 4}){sup +} complex forms through the bidentate carboxylate binding to U(VI). In the UO{sub 2}(GH{sub 3})(aq) complex, hydroxyl-deprotonated gluconate (GH{sub 3}{sup 2-}) coordinates to U(VI) through the five-membered ring chelation. For the UO{sub 2}(GH{sub 3})(GH{sub 4}){sup -} complex, multiple coordination modes are suggested. These results are discussed in the context of trivalent and pentavalent actinide complexation by gluconate.
Date: January 5, 2009
Creator: Zhang, Zhicheng; Helms, G.; Clark, S. B.; Tian, Guoxin; Zanonato, PierLuigi & Rao, Linfeng
Partner: UNT Libraries Government Documents Department

Chemical speciation of strontium, americium, and curium in high level waste: Predictive modeling of phase partitioning during tank processing. 1998 annual progress report

Description: 'In this research program, Pacific Northwest National Laboratory (PNNL) and Florida State University (FSU) are investigating the speciation of Sr and Am/Cm in the presence of selected organic chelating agents (ethylenediaminetetraacetic acid (EDTA), N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA), nitrilotriacetic acid (NTA), and iminodiacetic acid (IDA)) over ranges of hydroxide, carbonate, ionic strength, and competing metal ion concentrations present in high level waste tanks. The fundamental understanding of chemical speciation reactions gained from these studies is also used to propose methodologies for removal of Sr and Am/Cm from organic chelates present in high level tank waste, via competition, displacement or other reactions, without the need for the development of costly and potentially hazardous organic destruction technologies.'
Date: June 1, 1998
Creator: Felmy, A. R.
Partner: UNT Libraries Government Documents Department

Toward understanding the thermodynamics of TALSPEAK process. Medium effects on actinide complexation

Description: The ingenious combination of lactate and diethylenetriamine-N,N,N’,N”,N”-pentaacetic acid (DTPA) as an aqueous actinide-complexing medium forms the basis of the successful separation of americium and curium from lanthanides known as the TALSPEAK process. While numerous reports in the prior literature have focused on the optimization of this solvent extraction system, considerably less attention has been devoted to the understanding of the basic thermodynamic features of the complex fluids responsible for the separation. The available thermochemical information of both lactate and DTPA protonation and metal complexation reactions are representative of the behavior of these ions under idealized conditions. Our previous studies of medium effects on lactate protonation suggest that significant departures from the speciation predicted based on reported thermodynamic values should be expected in the TALSPEAK aqueous environment. Thermodynamic parameters describing the separation chemistry of this process thus require further examination at conditions significantly removed from conventional ideal systems commonly employed in fundamental solution chemistry. Such thermodynamic characterization is the key to predictive modelling of TALSPEAK. Improved understanding will, in principle, allow process technologists to more efficiently respond to off-normal conditions during large scale process operation. In this report, the results of calorimetric and potentiometric investigations of the effects of aqueous electrolytes on the thermodynamic parameters for lactate protonation and lactate complexation of americium and neodymium will be presented. Studies on the lactate protonation equilibrium will clearly illustrate distinct thermodynamic variations between strong electrolyte aqueous systems and buffered lactate environment.
Date: July 1, 2009
Creator: Zalupski, Peter R; Martin, Leigh R; Nash, Ken; Nakamura, Yoshinobu & Yamamoto, Masahiko
Partner: UNT Libraries Government Documents Department

Actinide Targets for Neutron Cross Section Measurements

Description: The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from "minor" actinides that currently have poorly known or in some cases not measured (n,?) and (n,f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 239Pu, 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.
Date: October 1, 2006
Creator: Baker, John D. & McGrath, Christopher A.
Partner: UNT Libraries Government Documents Department

Separation of Minor Actinides from Lanthanides by Dithiophosphinic Acid Extractants

Description: The selective extraction of the minor actinides (Am(III) and Cm(III)) from the lanthanides is an important part of advanced reprocessing of spent nuclear fuel. This separation would allow the Am/Cm to be fabricated into targets and recycled to a reactor and the lanthanides to be dispositioned. This separation is difficult to accomplish due to the similarities in the chemical properties of the trivalent actinides and lanthanides. Research efforts at the Idaho National Laboratory have identified an innovative synthetic pathway yielding new regiospecific dithiophosphinic acid (DPAH) extractants. The synthesis provides DPAH derivatives that can address the issues concerning minor actinide separation and extractant stability. For this work, two new symmetric DPAH extractants have been prepared. The use of these extractants for the separation of minor actinides from lanthanides will be discussed.
Date: September 1, 2008
Creator: Peterman, D. R.; Greenhalgh, M. R.; Tillotson, R. D.; Klaehn, J. R.; Harrup, M. K.; Luther, T. A. et al.
Partner: UNT Libraries Government Documents Department

United States Transuranium and Uranium Registries. Annual report October 1, 1994 - September 30, 1995

Description: The United States Transuranium and Uranium Registries (USTUR) comprise a human tissue research program studying the deposition, biokinetics and dosimetry of the actinide elements in humans with the primary goals of providing data fundamental to the verification, refinement, or future development of radiation protection standards for these and other radionuclides, and of determining possible bioeffects on both a macro and subcellular level attributable to exposure to the actinides. This report covers USTUR activities during the year from October 1994 through September 1995.
Date: July 1, 1996
Creator: Kathren, R.L.; Harwick, L.A. & Markel, M.J.
Partner: UNT Libraries Government Documents Department

United States Transuranium and Uranium Registries. Annual report February 1, 2000--January 31, 2001

Description: The United States Transuranium and Uranium Registries (USTUR) comprise a human tissue research program studying the deposition, biokinetics and dosimetry of the actinide elements in humans with the primary goals of providing data fundamental to the verification, refinement, or future development of radiation protection standards for these and other radionuclides, and of determining possible bioeffects on both a macro and subcellular level attributable to exposure to the actinides. This report covers USTUR activities during the year from February 2000 through January 2001.
Date: July 1, 2001
Creator: Ehrhart, Susan M. (ed.) & Filipy, Ronald E. (ed.)
Partner: UNT Libraries Government Documents Department

United States Transuranium and Uranium Registries. Annual report February 1, 2001--January 31, 2002

Description: This report documents the activities of the United States Transuranium and Uranium Registries (USTUR) from February 2001 through January 2002. Progress in continuing collaborations and several new collaborations is reviewed.
Date: July 1, 2002
Creator: Ehrhart, Susan M. & Filipy, Ronald E. (ed)
Partner: UNT Libraries Government Documents Department

Final Technical Progress Report Long term risk from actinides in the environment: Modes of mobility

Description: The key source of uncertainty in assessing actinide mobility is the relative importance of transport by: (1) wind erosion, (2) water erosion, and (3) vertical migration. Each of these three processes depends on several environmental factors and they compete with one another. A scientific assessment of the long-term risks associated with actinides in surface soils depends on better quantifying each of these three modes of mobility. The objective from our EMSP study was to quantify the mobility of soil actinides by wind erosion, water erosion, and vertical migration at three semiarid sites where actinide mobility is a key technical, social and legal issue. This EMSP project was the first to evaluate all three factors at a site. The approach has been to investigate both short- and long-term issues based on field and lab studies and model comparisons. Our results demonstrate the importance of incorporating threshold responses into a modeling framework that accounts for environmental factors and natural disturbances that trigger large changes in actinide mobility. The study measured erosional losses of sediment and fallout cesium (an actinide analogue) from field plots located near WIPP in 1998. The results highlight the large effect of burning as a disturbance on contaminant transport and mobility via runoff and erosion. The results show that runoff, erosion, and actinide transport are (1) strongly site specific-differences in radionuclide transport between WIPP and Rocky Flats differed by a factor of twelve because of soil and vegetation differences, and (2) are strongly impacted by disturbances such as fire, which can increase runoff, erosion, and actinide transport by more than an order of magnitude. In addition, a laboratory experiment using soil columns was conducted to investigate the vertical transport of contaminants in sandy soils. Nine columns of soil collected from the vicinity of the WIPP site were prepared. The ...
Date: March 22, 2002
Creator: Kirchner, Thomas B.
Partner: UNT Libraries Government Documents Department

Bridging the Gap in the Chemical Thermodynamic Database for Nuclear Waste Repository: Studies of the Effect of Temperature on Actinide Complexation

Description: Recent results of thermodynamic studies on the complexation of actinides (UO{sub 2}{sup 2+}, NpO{sub 2}{sup +} and Pu{sup 4+}) with F{sup -}, SO{sub 4}{sup 2-} and H{sub 2}PO{sub 4}{sup -}/HPO{sub 4}{sup 2-} at elevated temperatures are reviewed. The data indicate that, for all systems except the 1:1 complexation of Np(V) with HPO{sub 4}{sup 2-}, the complexation of actinides is enhanced by the increase in temperature. The enhancement is primarily due to the increase in the entropy term (T{Delta}S) that exceeds the increase in the enthalpy ({Delta}H) as the temperature is increased. These data bridge the gaps in the chemical thermodynamic database for nuclear waste repository where the temperature could remain significantly higher than 25 C for a long time after the closure of the repository.
Date: December 21, 2009
Creator: Rao, Linfeng; Tian, Guoxin; Xia, Yuanxian; Friese, Judah I.; Zanonato, PierLuigi & Di Bernardo, Plinio
Partner: UNT Libraries Government Documents Department

Chemical properties of the transactinide elements studied inliquid phase with SISAK

Description: This article starts with a review of the current SISAKliquid-liquid extraction system, as used after the physical preseparatorBGS at LBNL for chemical studies of transactinide elements. Emphasis willbe on new additions and developments. Then the possibilities offered bythe new TASCA separator at GSI and the use of actinide targets at bothGSI and LBNL are discussed with respect to future SISAK transactinideexperiments. Finally, current and future liquid-liquid extraction systemsfor studying elements Rf up to Hs are discussed.
Date: May 1, 2007
Creator: Omtvedt, J.P.; Alstad, J.; Bjornstad, T.; Dullmann, Ch.E.; Gregorich, K.E.; Hoffman, D.C. et al.
Partner: UNT Libraries Government Documents Department

Characterization of a mixed salt of 1-hydroxy-pyridin-2-one Pu(IV)complexes

Description: Most expert analyses of the projected world energy needs show utilization of nuclear energy will be essential for the next few decades, and hence the need to support this technology grows. But as one measure of the supporting science base of this field, as of December 2006, only 25 Pu containing structures were in the Cambridge Structural Database, as compared to 21,807 for Fe. A comparison of the rate of addition to this knowledge base reveals that approximately 500 Fe structures are registered with the Cambridge Structural Database every year, while in the same period only two or three Pu crystal structures are published. A continuing objective of this laboratory has been the development of new sequestering agents for actinide decorporation and selective extractions. This effort has been based on similarities in the properties of Pu(IV) and Fe(III), and the chelating groups in microbial Fe(III) sequestering agents, siderophores. The HOPO ligands (Figure 1) are one such class of chelating group which have been investigated as selective actinide extractants.
Date: January 9, 2007
Creator: Gorden, Anne E.V.; Xu, Jide; Szigethy, Geza; Oliver, Allen; Shuh,David K. & Raymond, Kenneth N.
Partner: UNT Libraries Government Documents Department

Calculational Study on the Compounds Np3M, Am3M, and on the System Pu-Am

Description: Spin-polarized relativistic density functional theory has been employed for the study of the electronic and magnetic structures for the compounds Np{sub 3}M and Am{sub 3}M (M = Al; Ga; In) and their comparison with plutonium's alloys Pu{sub 3}M has been made. It has been found that of the three actinides (Np, Pu, Am) only plutonium has its FCC structure essentially more stable after alloying with aforementioned elements. Apart from that, the electronic and magnetic structures for the system Pu-Am presented by three different compounds: Pu{sub 3}Am, PuAm, and PuAm{sub 3} have been investigated. Their magnetic structures have been found to be too robust in comparison with the experimental fact that magnetism in Pu-Am system depends strongly on the percentage of the americium in the alloy. One possible explanation consists in the overestimation of the spin splitting and in the disregarding of orbital dependence of the exchange-correlation potential.
Date: September 7, 2005
Creator: Kutepov, A L
Partner: UNT Libraries Government Documents Department

The Metabolic Properties of the Fission Products and Actinide Elements

Description: An investigation of the assimilation, distribution, retention, an excretion of the fission products and actinide elements in the rat has been conducted at the Crocker Radiation Laboratory, University of California, Berkeley, California. These studies were initiated October 15, 1942, and are continuing at the present time. An extensive survey has been made of the metabolism of twenty-two different radio elements in the rat.
Date: March 1, 1948
Creator: Hamilton M.D., J.G.
Partner: UNT Libraries Government Documents Department

A moving target: responding to magnetic and structural disorder in lanthanide- and actinide-based superconductors

Description: The effects of various chemical substitutions and induced lattice disorder in the Ce- and Pu-based 115 superconductors are reviewed, with particular emphasis on results from x-ray absorption fine structure (XAFS) measurements. The PuCoGa{sub 5} system offers the opportunity to follow changes in magnetic and electronic properties due to lattice disorder as a function of time in the same samples, in addition to the more traditional approach of perturbing the superconducting state through chemical substitutions. The reviewed work establishes a baseline for such future studies by determining the intrinsic lattice order in the 115 system, successfully understanding disorder as introduced through chemical substitutions in the Ce-based 115s, and beginning to explore the surprisingly large role of self-irradiation damage directly on the PuCoGa{sub 5} lattice. These studies lay the foundation for the harder future work toward measuring chemical substitutions in PuCoGa{sub 5}, correlating effects with non-Fermi liquid behavior, and obtaining a better structural picture of the distortions induced by {alpha}-decay of the plutonium nucleus.
Date: February 10, 2010
Creator: Booth, Corwin H.; Bauer, Eric D. & Mitchel, Jeremy N.
Partner: UNT Libraries Government Documents Department

TRANSURANIUM QUARTERLY PROGRESS REPORT FOR PERIOD ENDING FEBRUARY 28, 1963

Description: The development of separation processes for the transuranium elements, process equipment development, HFIR target fabrication development, design of the TRU Facility, design of development facilities, corrosion studies, and analytical research and development studies are reported. (auth)
Date: October 1, 1963
Creator: Burch, W.D. comp.
Partner: UNT Libraries Government Documents Department