Science.gov

Sample records for americium isotopes

  1. The Most Useful Actinide Isotope: Americium-241.

    ERIC Educational Resources Information Center

    Navratil, James D.; And Others

    1990-01-01

    Reviewed is the discovery, nuclear and chemical properties, and uses of an isotope of Americium (Am-241). Production and separation techniques used in industry are emphasized. Processes are illustrated in flow sheets. (CW)

  2. Updated Evaluations for Americium Isotopes

    SciTech Connect

    Brown, D A; Pruet, J

    2005-09-22

    Here we describe evaluations for Am isotopes that will be included in the next release of ENDL. Current ENDL99 evaluations for these isotopes are quite outdated and almost entirely undocumented. Because Am is important for several DNT applications, and because quality evaluations are either readily available or easily calculated, the effort to update ENDL seems warranted. Results from good existing evaluations are adopted whenever possible. To this end we devote the next section of this report to a consideration of the availability of evaluations The quality of different evaluations as well as comparisons against experiments are also presented and used to motivate our choice of adopted data sets. Plans for modifying and improving adopted evaluations are also discussed. For {sup 240}Am there are no existing evaluations. To fill this gap, we are providing a new Am evaluation based on calculations with the statistical model reaction codes TALYS and EMPIRE. This evaluation is described below. The ENDF/B-VI formatted file containing this evaluation is given in the appendix.

  3. Americium

    NASA Astrophysics Data System (ADS)

    Runde, Wolfgang H.; Schulz, Wallace W.

    Americium, element 95, was discovered in 1944-45 by Seaborg et al. (1950) at the Metallurgical Laboratory of the University of Chicago as a product of the irradiation of plutonium with neutrons: 239{Pu}( n,γ )^{240} Put( n,γ )^{241} Pu → - β ^-}^{241}{Am} This reaction is still the best method for the production of pure 241Am. In post-World War II work at the University of Chicago, Cunningham isolated Am(OH)3 and measured the first absorption spectrum of the Am3+ aquo ion (Cunningham, 1948). By the 1950s, the major center for americium chemistry research in the world was at Los Alamos. Since the 1970s, the majority of publications on americium have come from researchers in the former USSR and West Germany. Extensive reviews of americium chemistry can be found in Freeman and Keller (1985), Gmelin (1979), Penneman and Asprey (1955), and Schulz (1976).

  4. Americium

    SciTech Connect

    Smith, James L

    2012-06-01

    The element americium marks the end of interesting behavior in the periodic table. I will talk about how this was predicted by Johansson and Rosengren and demonstrated by me. I will talk about other questions of localization.

  5. Rapid, quantitative analysis of americium, curium and plutonium isotopes in Hanford samples using extraction chromatography and precipitation plating

    SciTech Connect

    Kaye, J.H.; Strebin, R.S.; Orr, R.D.

    1994-04-01

    Recently developed methods for the rapid, quantitative analysis of americium (Am), curium (Cm), and plutonium (Pu) isotopes in Hanford soil, sludge, and waste-tank samples are described. After dissolution, dilutions are made as necessary based on alpha-energy analysis of a small aliquot of the original solution. isotopic tracers are then added and Am-Cm and Pu are separated by extraction chromatography, coprecipitated with neodymium fluoride, and counted. Examples of alpha spectra are given, and results obtained for Hanford sludge samples are presented.

  6. Cesium, americium and plutonium isotopes in ground level air of vilnius

    NASA Astrophysics Data System (ADS)

    Lujaniene, G.; Šapolaite, J.; Remeikis, V.; Lujanas, V.; Jermolajev, A.; Aninkevičius, V.

    2006-01-01

    Systematic observations of radionuclide composition and concentration in the atmosphere have been carried out at the Institute of Physics in Vilnius since 1963. Increases in activity concentration of radionuclides in the atmosphere were observed after nuclear weapon tests and the Chernobyl NPP accident. At present the radiation situation in Lithuania is determined by two main sources of radionuclides, forest fire and resuspension products transferred from highly polluted region of the Ukraine and Belarus. The activity concentrations of 137Cs were measured in two to three days samples while plutonium and americium in monthly samples. The extremely high activity concentrations of 238Pu, 239,240Pu, 241Am determined in the atmosphere during the Chernobyl accident can be explained by transport of “hot particles” of different composition. Activity concentration in 1995 2003 of 241Am and 239,240Pu isotopes ranged from 0.3 to 500 and from 1 to 500 nBq/m3, respectively. 238Pu/239,240Pu activity ratio in measured samples differs from 0.03 to 0.45. A decrease in 240Pu/239Pu atomic ratio from 0.30 to 0.19 was observed in 1995 2003.

  7. Neutron capture and neutron-induced fission experiments on americium isotopes with DANCE

    SciTech Connect

    Jandel, M.; Bredeweg, T. A.; Fowler, M. M.; Bond, E. M.; Couture, A.; Haight, R. C.; Keksis, A. L.; O'Donnell, J. M.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Stoyer, M. A.; Wu, C. Y.; Becker, J. A.; Haslett, R. J.; Henderson, R. A.

    2009-01-28

    Neutron capture cross section data on Am isotopes were measured using the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory. The neutron capture cross section was determined for {sup 241}Am for neutron energies between thermal and 320 keV. Preliminary results were also obtained for {sup 243}Am for neutron energies between 10 eV and 250 keV. The results on concurrent neutron-induced fission and neutron-capture measurements on {sup 242m}Am will be presented where the fission events were actively triggered during the experiments. In these experiments, a Parallel-Plate Avalanche Counter (PPAC) detector that surrounds the target located in the center of the DANCE array was used as a fission-tagging detector to separate (n,{gamma}) events from (n,f) events. The first direct observation of neutron capture on {sup 242m}Am in the resonance region in between 2 and 9 eV of the neutron energy was obtained.

  8. Neutron capture and neutron-induced fission experiments on americium isotopes with DANCE

    SciTech Connect

    Jandel, Marian

    2008-01-01

    Neutron capture cross section data on Am isotopes were measured using the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory. The neutron capture cross section was determined for {sup 241}Am for neutron energies between thermal and 320 keV. Preliminary results were also obtained for {sup 243}Am for neutron energies between 35 eV and 200 keV. The results on concurrent neutron-induced fission and neutron-capture measurements on {sup 242m}Am will be presented, where the fission events were actively triggered during the experiments. In these experiments, the Parallel-Plate Avalanche Counter (PPAC) detector that surrounds the target located in the center of the DANCE array was used as a fission-tagging detector to separate (n,{gamma}) from (n,f) events. The first evidence of neutron capture on {sup 242m}Am in the resonance region in between 2 and 9 eV of the neutron energy was obtained.

  9. Determination of Atto- to Femtogram Levels of Americium and Curium Isotopes in Large-Volume Urine Samples by Compact Accelerator Mass Spectrometry.

    PubMed

    Dai, Xiongxin; Christl, Marcus; Kramer-Tremblay, Sheila; Synal, Hans-Arno

    2016-03-01

    Ultralow level analysis of actinides in urine samples may be required for dose assessment in the event of internal exposures to these radionuclides at nuclear facilities and nuclear power plants. A new bioassay method for analysis of sub-femtogram levels of Am and Cm in large-volume urine samples was developed. Americium and curium were co-precipitated with hydrous titanium oxide from the urine matrix and purified by column chromatography separation. After target preparation using mixed titanium/iron oxides, the final sample was measured by compact accelerator mass spectrometry. Urine samples spiked with known quantities of Am and Cm isotopes in the range of attogram to femtogram levels were measured for method evaluation. The results are in good agreement with the expected values, demonstrating the feasibility of compact accelerator mass spectrometry (AMS) for the determination of minor actinides at the levels of attogram/liter in urine samples to meet stringent sensitivity requirements for internal dosimetry assessment. PMID:26822907

  10. MODELING AND FISSION CROSS SECTIONS FOR AMERICIUM.

    SciTech Connect

    ROCHMAN, D.; HERMAN, M.; OBLOZINSKY, P.

    2005-05-01

    This is the final report of the work performed under the LANL contract on the modeling and fission cross section for americium isotopes (May 2004-June 2005). The purpose of the contract was to provide fission cross sections for americium isotopes with the nuclear reaction model code EMPIRE 2.19. The following work was performed: (1) Fission calculations capability suitable for americium was implemented to the EMPIRE-2.19 code. (2) Calculations of neutron-induced fission cross sections for {sup 239}Am to {sup 244g}Am were performed with EMPIRE-2.19 for energies up to 20 MeV. For the neutron-induced reaction of {sup 240}Am, fission cross sections were predicted and uncertainties were assessed. (3) Set of fission barrier heights for each americium isotopes was chosen so that the new calculations fit the experimental data and follow the systematics found in the literature.

  11. RECOVERY OF AMERICIUM

    DOEpatents

    Ader, M.; Hyman, H.H.

    1960-04-26

    A process is given for separating americium and plutonium and recovering the americium. Plutonium is extracted from a solution containing plutonium and americium with a water-insoluble solvent, and americium is precipitated from the aqueous phase by adding a ferric salt and an alkali metal hydroxide thereto. The precipitate may then be dissolved in hydrochloric acid and the ferric salt extracted from the americium with an organlc solvent.

  12. Neutron production in several americium compounds

    SciTech Connect

    Shores, E. F.

    2004-01-01

    Americium, like other alpha emitting actinides, may indirectly produce neutrons when combined with light target materials. These (alpha,n) reaction neutrons, along with well known photon lines, have been an advantage of the {sup 241}Am isotope for diverse applications such as radiography, thickness gauges, neutron sources, and even common household smoke detectors. To characterize these sources, the SOURCES code was used to calculate neutron yields and spectra from {sup 241}Am metal, americium oxide, and americium aluminum alloys. Such information may be used as source terms for future transport problems (e.g. shielding calculations). Table 1 contains neutron yields for six americium configurations. The metal, oxides, and alloys were run as homogeneous problems while the interface case was run in both two- and three-region interface modes.

  13. New Fecal Method for Plutonium and Americium

    SciTech Connect

    Maxwell, S.L. III

    2000-06-27

    A new fecal analysis method that dissolves plutonium oxide was developed at the Westinghouse Savannah River Site. Diphonix Resin (Eichrom Industries), is used to pre-concentrate the actinides from digested fecal samples. A rapid microwave digestion technique is used to remove the actinides from the Diphonix Resin, which effectively extracts plutonium and americium from acidic solutions containing hydrofluoric acid. After resin digestion, the plutonium and americium are recovered in a small volume of nitric acid that is loaded onto small extraction chromatography columns, TEVA Resin and TRU Resin (Eichrom Industries). The method enables complete dissolution of plutonium oxide and provides high recovery of plutonium and americium with good removal of thorium isotopes such as thorium-228.

  14. Americium recovery from reduction residues

    DOEpatents

    Conner, W.V.; Proctor, S.G.

    1973-12-25

    A process for separation and recovery of americium values from container or bomb'' reduction residues comprising dissolving the residues in a suitable acid, adjusting the hydrogen ion concentration to a desired level by adding a base, precipitating the americium as americium oxalate by adding oxalic acid, digesting the solution, separating the precipitate, and thereafter calcining the americium oxalate precipitate to form americium oxide. (Official Gazette)

  15. The New Element Americium (Atomic Number 95)

    DOE R&D Accomplishments Database

    Seaborg, G.T.; James, R.A.; Morgan, L.O.

    1948-01-01

    Several isotopes of the new element 95 have been produced and their radiations characterized. The chemical properties of this tripositive element are similar to those of the typical tripositive lanthanide rare-earth elements. Element 95 is different from the latter in the degree and rate of formation of certain compounds of the complex ion type, which makes possible the separation of element 95 from the lanthanide rare-earths. The name americium (after the Americas) and the symbol Am are suggested for the element on the basis of its position as the sixth member of the actinide rare-earth series, analogous to europium, Eu, of the lanthanide series.

  16. SEPARATION OF AMERICIUM FROM PROMETHIUM

    DOEpatents

    Pressly, R.E.

    1959-07-01

    Promethium-147 is separated from americium in acidic aqueous solution by adding fluosilicic acid to the solution, heating the solution to form a promethium precipitate and separating the precipitate from solution. The precipitate is then re-dissolved by ihe addition of boric acid and nitric acid, and re-precipitated by the addition of fluosilicic acid. This procedure is repeated six or more times to obtain a relatively americium-free promeihium precipitate. Americium may be separately recovered from the supernatant liquids. This process is applicable to the recovery of promethium from fission-product solutions which have been allowed to decay for a period of two to four years.

  17. SEPARATION OF CURIUM AND AMERICIUM

    DOEpatents

    Fields, P.R.; Isaac, N.M.

    1962-02-20

    Curium and americium are contained in an anhydrous molten salt medium having a low melting point. Curium is preferentially extracted from the molten salt by a hot organic solvent containing preferably less than 10% alkyl phosphate. (AEC)

  18. I. Nuclear Production Reaction and Chemical Isolation Procedure for Americium-240 II. New Superheavy Element Isotopes: Plutonium-242(Calcium-48,5n)(285)114

    NASA Astrophysics Data System (ADS)

    Ellison, Paul Andrew

    2011-12-01

    Part I discusses the study of a new nuclear reaction and chemical separation procedure for the production of 240Am. Thin 242Pu, natTi, and natNi targets were coincidently activated with protons from the 88-Inch Cyclotron, producing 240Am, 48V, and 57Ni, respectively. The radioactive decay of these isotopes was monitored using high-purity Ge gamma ray detectors in the weeks following irradiation. The excitation function for the 242 Pu(p, 3n)240Am nuclear reaction was measured to be lower than theoretical predictions, but high enough to be the most viable nuclear reaction for the large-scale production of 240 Am. Details of the development of a chemical separation procedure for isolating 240Am from proton-irradiated 242Pu are discussed. The separation procedure, which includes two anion exchange columns and two extraction chromatography columns, was experimentally investi- gated using tracer-level 241Am, 239Pu, and model proton-induced fission products 95Zr, 95Nb, 125Sb, and 152Eu. The separation procedure was shown to have an Am/Pu separation factor of >2x10 7 and an Am yield of ˜70%. The separation procedure was found to purify the Am sample from >99.9% of Eu, Zr, Nb, and Sb. The procedure is well suited for the processing of ˜1 gram of proton-irradiated 242Pu to produce a neutron-induced fission target consisting of tens of nanograms of 240Am. Part II describes the use of the Berkeley Gas-filled Separator at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron for the study of the 242Pu(48Ca,5n)285114 nuclear re- action. The new, neutron-deficient, superheavy element isotope 285114 was produced in 48Ca irradiations of 242Pu targets at a center-of-target beam energy of 256 MeV ( E* = 50 MeV). The alpha decay of 285114 was followed by the sequential alpha decay of four daughter nuclides, 281Cn, 277Ds, 273Hs, and 269 Sg. 265Rf was observed to decay by spontaneous fission. The measured alpha-decay Q-values were compared with those from a macroscopic

  19. Plutonium and americium separation from salts

    DOEpatents

    Hagan, Paul G.; Miner, Frend J.

    1976-01-01

    Salts or materials containing plutonium and americium are dissolved in hydrochloric acid, heated, and contacted with an alkali metal carbonate solution to precipitate plutonium and americium carbonates which are thereafter readily separable from the solution.

  20. Phonon dynamics of americium telluride

    NASA Astrophysics Data System (ADS)

    Arya, B. S.; Aynyas, Mahendra; Ahirwar, Ashok K.; Sanyal, S. P.

    2013-06-01

    We report for the first time the complete phonon dispersion curves for Americium telluride (AmTe) using a breathing shell models (BSM) to establish their predominant ionic nature. The results obtained in the present study show the general features of the phonon spectrum. We could not compare our results with the experimental measurements as they are not available so far. We emphasize the need of neutron scattering measurements to compare our results. We also report, for the first time specific heat for this compound.

  1. Lifetime followup of the 1976 americium accident victim: (Final report)

    SciTech Connect

    Breitenstein, B.D. Jr.; Palmer, H.E.

    1988-05-01

    This report describes the 11 year medical course of Harold R. McCluskey, a Hanford nuclear chemical operator, who, at age 64, was involved in an accident in an americium recovery facility in August 1976. As a result of the accident, he was heavily contaminated with americium (Am-241), sustained a substantial internal deposition of this isotope, and was burned with concentrated nitric acid and injured by flying debris about the face and neck. The immediate and long-term medical care is summarized, including decontamination procedures, chelation therapy, and routine and special clinical laboratories studies. The estimates of the operator's Am-241 deposition, post accident and during the remainder of his life and the special techniques and equipment used to make the estimates, are reported. Post-accident, the total amount of Am-241 excreted in his urine and feces was 41 MBq (1.1 mCi). He died of complications of chronic coronary artery disease on August 17, 1987. 20 refs., 2 figs.

  2. Americium thermodynamic data for the EQ3/6 database

    SciTech Connect

    Kerrisk, J.F.

    1984-07-01

    Existing thermodynamic data for aqueous and solid species of americium have been reviewed and collected in a form that can be used with the EQ3/6 database. Data that are important in solubility calculations for americium at a proposed Yucca Mountain nuclear waste repository were emphasized. Conflicting data exist for americium complexes with carbonates. Essentially no data are available for americium solids or complexes at temperatures greater than 25{sup 0}C. 17 references, 4 figures.

  3. Americium separations from high salt solutions

    SciTech Connect

    Mary E. Barr; Gordon D. Jarvinen; Louis D. Schulte; Peter C. Stark; Rebecca M. Chamberlin; Kent D. Abney; Thomas E. Ricketts; Yvette E. Valdez; Richard A. Bartsch

    2000-03-01

    Americium (III) exhibits an unexpectedly high affinity for anion-exchange material from the high-salt evaporator bottoms solutions--an effect which has not been duplicated using simple salt solutions. Similar behavior is observed for its lanthanide homologue, Nd(III), in complex evaporator bottoms surrogate solutions. There appears to be no single controlling factor--acid concentration, total nitrate concentration or solution ionic strength--which accounts for the approximately 2-fold increase in retention of the trivalent ions from complex solutions relative to simple solutions. Calculation of species activities (i.e., water, proton and nitrate) in such concentrated mixed salt solutions is difficult and of questionable accuracy, but it is likely that the answer to forcing formation of anionic nitrate complexes of americium lies in the relative activities of water and nitrate. From a practical viewpoint, the modest americium removal needs (ca. 50--75%) from nitric acid evaporator bottoms allow sufficient latitude for the use of non-optimized conditions such as running existing columns filled with older, well-used Reillex HPQ. Newer materials, such as HPQ-100 and the experimental bifunctional resins, which exhibit higher distribution coefficients, would allow for either increased Am removal or the use of smaller columns. It is also of interest that one of the experimental neutral-donor solid-support extractants, DHDECMP, exhibits a similarly high level of americium (total alpha) removal from EV bottoms and is much less sensitive to total acid content than commercially-available material.

  4. Portable, high intensity isotopic neutron source provides increased experimental accuracy

    NASA Technical Reports Server (NTRS)

    Mohr, W. C.; Stewart, D. C.; Wahlgren, M. A.

    1968-01-01

    Small portable, high intensity isotopic neutron source combines twelve curium-americium beryllium sources. This high intensity of neutrons, with a flux which slowly decreases at a known rate, provides for increased experimental accuracy.

  5. Status of Americium-241 recovery at Rocky Flats Plant

    SciTech Connect

    Knighton, J.B.; Hagan, P.G.; Navratil, J.D.; Thompson, G.H.

    1981-01-01

    This paper is presented in two parts: Part I, Molten Salt Extraction of Americium from Molten Plutonium Metal, and Part II, Aqueous Recovery of Americium from Extraction Salts. The Rocky Flats recovery process used for waste salts includes (1) dilute hydrochloric acid dissolution of residues; (2) cation exchange to convert from the chloride to the nitrate system and to remove gross amounts of monovalent impurities; (3) anion exchange separation of plutonium; (4) oxalate precipitation of americium; and (5) calcination of the oxalate at 600/sup 0/C to yield americium oxide. The aqueous process portion describes attempts to improve the recovery of americium. The first part deals with modifications to the cation exchange step; the second describes development of a solvent extractions process that will recovery americium from residues containing aluminium as well as other common impurities. Results of laboratory work are described. 3 figures, 6 tables. (DP)

  6. Final Radiological Assessment of External Exposure for CLEAR-Line Americium Recovery Operations

    SciTech Connect

    Davis, Adam C.; Belooussova, Olga N.; Hetrick, Lucas Duane

    2014-11-12

    Los Alamos National Laboratory is currently planning to implement an americium recovery program. The americium, ordinarily isotopically pure 241Am, would be extracted from existing Pu materials, converted to an oxide and shipped to support fabrication of americium oxide-beryllium neutron sources. These operations would occur in the currently proposed Chloride Extraction and Actinide Recovery (CLEAR) line of glove boxes. This glove box line would be collocated with the currently-operational Experimental Chloride Extraction Line (EXCEL). The focus of this document is to provide an in-depth assessment of the currently planned radiation protection measures and to determine whether or not further design work is required to satisfy design-goal and ALARA requirements. Further, this document presents a history of americium recovery operations in the Department of Energy and high-level descriptions of the CLEAR line operations to provide a basis of comparison. Under the working assumptions adopted by this study, it was found that the evaluated design appears to mitigate doses to a level that satisfies the ALARA-in-design requirements of 10 CFR 835 as implemented by the Los Alamos National Laboratory procedure P121. The analyses indicate that extremity doses would also meet design requirements. Dose-rate calculations were performed using the radiation transport code MCNP5 and doses were estimated using a time-motion study developed in consort with the subject matter expert. A copy of this report and all supporting documentation are located on the Radiological Engineering server at Y:\\Rad Engineering\\2013 PROJECTS\\TA-55 Clear Line.

  7. oxidation of americium(iii) and the stability of americium(iv) and americium(vi) in solutions of sulfuric and perchloric acids

    SciTech Connect

    Milyukova, M.S.; Litvina, M.N.; Myasoedov, B.F.

    1986-07-01

    The oxidation of weighable amounts of americium in solutionsof sulfuric and perchloric acids was investigated by a spectrophotometric method. The stability of americium(IV) and (VI) in mineral acids was studied. A method was developed for the production of tetravalent americium in solutions of 0.1-3 M H/sub 2/SO/sub 4/ and 0.1-1 M HClO/sub 4/, containing potassium phosphotungstate K/sub 10/P/sub 2/W/sub 17/O/sub 61/ an an oxidizing mixture - a silver salt and ammonium persulfate.

  8. Surface complexation modeling of americium sorption onto volcanic tuff.

    PubMed

    Ding, M; Kelkar, S; Meijer, A

    2014-10-01

    Results of a surface complexation model (SCM) for americium sorption on volcanic rocks (devitrified and zeolitic tuff) are presented. The model was developed using PHREEQC and based on laboratory data for americium sorption on quartz. Available data for sorption of americium on quartz as a function of pH in dilute groundwater can be modeled with two surface reactions involving an americium sulfate and an americium carbonate complex. It was assumed in applying the model to volcanic rocks from Yucca Mountain, that the surface properties of volcanic rocks can be represented by a quartz surface. Using groundwaters compositionally representative of Yucca Mountain, americium sorption distribution coefficient (Kd, L/Kg) values were calculated as function of pH. These Kd values are close to the experimentally determined Kd values for americium sorption on volcanic rocks, decreasing with increasing pH in the pH range from 7 to 9. The surface complexation constants, derived in this study, allow prediction of sorption of americium in a natural complex system, taking into account the inherent uncertainty associated with geochemical conditions that occur along transport pathways. PMID:24963803

  9. Electron heat capacity and lattice properties of Americium

    NASA Astrophysics Data System (ADS)

    Povzner, A. A.; Filanovich, A. N.; Os'kina, V. A.; Volkov, A. G.

    2013-12-01

    The temperature dependence of the electron heat capacity of americium is calculated using the concepts on the electronic structure and magnetic properties of this element. The Debye temperature, the thermal expansion coefficient, and the bulk modulus of americium are determined on the basis of the results of calculations and experimental data on heat capacity.

  10. Removal of plutonium and americium from alkaline waste solutions

    DOEpatents

    Schulz, Wallace W.

    1979-01-01

    High salt content, alkaline waste solutions containing plutonium and americium are contacted with a sodium titanate compound to effect removal of the plutonium and americium from the alkaline waste solution onto the sodium titanate and provide an effluent having a radiation level of less than 10 nCi per gram alpha emitters.

  11. Density of simulated americium/curium melter feed solution

    SciTech Connect

    Rudisill, T.S.

    1997-09-22

    Vitrification will be used to stabilize an americium/curium (Am/Cm) solution presently stored in F-Canyon for eventual transport to Oak Ridge National Laboratory and use in heavy isotope production programs. Prior to vitrification, a series of in-tank oxalate precipitation and nitric/oxalic acid washes will be used to separate these elements and lanthanide fission products from the bulk of the uranium and metal impurities present in the solution. Following nitric acid dissolution and oxalate destruction, the solution will be denitrated and evaporated to a dissolved solids concentration of approximately 100 g/l (on an oxide basis). During the Am/Cm vitrification, an airlift will be used to supply the concentrated feed solution to a constant head tank which drains through a filter and an in-line orifice to the melter. Since the delivery system is sensitive to the physical properties of the feed, a simulated solution was prepared and used to measure the density as a function of temperature between 20 to 70{degrees} C. The measured density decreased linearly at a rate of 0.0007 g/cm3/{degree} C from an average value of 1.2326 g/cm{sup 3} at 20{degrees} C to an average value of 1.1973g/cm{sup 3} at 70{degrees} C.

  12. Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides

    SciTech Connect

    Horlait, Denis; Delahaye, Thibaud

    2014-09-15

    Americium oxides samples were characterized by X-ray diffraction (XRD) and Raman spectroscopy, with an emphasis on their structural behavior under oxidation and self-irradiation. Raman spectra of americium dioxide (AmO{sub 2}) and sesquioxide (Am{sub 2}O{sub 3}) were obtained for the first time. With the help of literature data on isostructural oxides, Raman signatures of Ia-3 C-type Am{sub 2}O{sub 3} and P-3m1 A-type Am{sub 2}O{sub 3} are identified. For AmO{sub 2,} a clear band is noted at 390 cm{sup −1}. Its nature is compared to that of the other actinide dioxides. Am{sub 2}O{sub 3} evolution under ambient conditions and against {sup 241}Am α self-irradiation was monitored by powder XRD. The sample, initially composed of A-type Am{sub 2}O{sub 3} as major phase as well as C2/m B-type and C-type structures as minor phases, progressively oxidizes to Fm-3m AmO{sub 2−δ} over a few months. On the basis of diffractogram refinements, evolutions of unit cell volumes caused by self-irradiation are also determined and discussed. - Graphical abstract: The evolution of americium oxide under ambient conditions was monitored using XRD (X-ray diffraction) and Raman spectroscopy. After a thermal treatment under reducing conditions, a polyphasic sample mainly composed of A- and C-type americium sesquioxides is evidenced by XRD and Raman spectroscopy. The sample then evolves through two processes: oxidation and self-irradiation. The first one provokes the progressive appearance of F-type americium dioxide while the initial phases disappear, whereas the main effect of the second is a structural swelling with time. - Highlights: • The first Raman spectroscopy measurements on americium oxides were performed. • Observed Am{sub 2}O{sub 3} Raman bands were identified thanks to data on analogue compounds. • AmO{sub 2} assumed T{sub 2g} band presents a shift compared to the actinide dioxide series. • Am{sub 2}O{sub 3} evolution under self-irradiation and oxidation was also

  13. RAPID METHOD FOR PLUTONIUM, AMERICIUM AND CURIUM IN VERY LARGE SOIL SAMPLES

    SciTech Connect

    Maxwell, S

    2007-01-08

    The analysis of actinides in environmental soil and sediment samples is very important for environmental monitoring. There is a need to measure actinide isotopes with very low detection limits. A new, rapid actinide separation method has been developed and implemented that allows the measurement of plutonium, americium and curium isotopes in very large soil samples (100-200 g) with high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin{reg_sign}, TRU Resin{reg_sign} and DGA-Resin{reg_sign} cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), americium (Am), and curium (Cm) using a single multistage column combined with alpha spectrometry. The method combines an acid leach step and innovative matrix removal using cerium fluoride precipitation to remove the difficult soil matrix. This method is unique in that it provides high tracer recoveries and effective removal of interferences with small extraction chromatography columns instead of large ion exchange resin columns that generate large amounts of acid waste. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.

  14. Higher Americium Oxidation State Research Roadmap

    SciTech Connect

    Mincher, Bruce J.; Law, Jack D.; Goff, George S.; Moyer, Bruce A.; Burns, Jon D.; Lumetta, Gregg J.; Sinkov, Sergey I.; Shehee, Thomas C.; Hobbs, David T.

    2015-12-18

    The partitioning of hexavalent Am from dissolved nuclear fuel requires the ability to efficiently oxidize Am(III) to Am(VI) and to maintain that oxidation state for a length of time sufficient to perform the separation. Several oxidants have been, or are being developed. Chemical oxidants include Ag-catalyzed ozone, Ag-catalyzed peroxydisulfate, Cu(III) periodate, and sodium bismuthate. Hexavalent americium has also now successfully been prepared by electrolysis, using functionalized electrodes. So-called auto-reduction rates of Am(VI) are sufficiently slow to allow for separations. However, for separations based on solvent extraction or ion exchange using organic resins, the high valence state must be maintained under the reducing conditions of the organic phase contact, and a holding oxidant is probably necessary. Until now, only Cu(III) periodate and sodium bismuthate oxidation have been successfully combined with solvent extraction separations. Bismuthate oxidation provided the higher DAm, since it acts as its own holding oxidant, and a successful hot test using centrifugal contactors was performed. For the other oxidants, Ag-catalyzed peroxydisulfate will not oxidize americium in nitric acid concentrations above 0.3 M, and it is not being further investigated. Peroxydisulfate in the absence of Ag catalysis is being used to prepare Am(V) in ion exchange work, discussed below. Preliminary work with Ag-catalyzed ozone has been unsuccessful for extractions of Am(VI) from 6.5 M HNO3, and only one attempt at extraction, also from 6.5 M HNO3, using the electrolytic oxidation has been attempted. However, this high acid concentration was based on the highest Am extraction efficiency using the bismuthate oxidant; which is only sparingly soluble, and thus the oxidation yield is based on bismuthate solubility. Lower acid concentrations may be sufficient with alternative oxidants and work with Ag-ozone, Cu(III) and electrolysis is on-going. Two non

  15. Frontiers of Chemistry for Americium and Curium

    DOE R&D Accomplishments Database

    Keller, O. L. Jr.

    1984-01-01

    The discoveries of americium and curium were made only after Seaborg had formulated his actinide concept in order to design the chemistry needed to separate them from irradiated /sup 239/Pu targets. Their discoveries thus furnished the first clear-cut evidence that the series exists and justified Seaborg`s bold assumption that even though Th and Pa appeared to presage a following 6d series, the pattern established by the periodic table after Cs and Ba would be repeated exactly after Fr and Ra. That is to say, a new 5f element rare earth series (the actinides) would follow Ac in the same way the 4f rare earth series (the lanthanides) follows La. The consequences of the resulting half-filled 5f/sup 7/ shell at Cm were originally presented by Seaborg as a test of his hypothesis. Recent research is outlined that substantiates Seaborg`s predictions in new and definitive ways.

  16. Frontiers of chemistry for americium and curium

    SciTech Connect

    Keller, O.L. Jr.

    1984-01-01

    The discoveries of americium and curium were made only after Seaborg had formulated his actinide concept in order to design the chemistry needed to separate them from irradiated /sup 239/Pu targets. Their discoveries thus furnished the first clear-cut evidence that the series exists and justified Seaborg's bold assumption that even though Th and Pa appeared to presage a following 6d series, the pattern established by the periodic table after Cs and Ba would be repeated exactly after Fr and Ra. That is to say, a new 5f element rare earth series (the actinides) would follow Ac in the same way the 4f rare earth series (the lanthanides) follows La. The consequences of the resulting half-filled 5f/sup 7/ shell at Cm were originally presented by Seaborg as a test of his hypothesis. Recent research is outlined that substantiates Seaborg's predictions in new and definitive ways. 15 references, 4 figures.

  17. PROCESS FOR SEPARATING AMERICIUM AND CURIUM FROM RARE EARTH ELEMENTS

    DOEpatents

    Baybarz, R.D.; Lloyd, M.H.

    1963-02-26

    This invention relates to methods of separating americium and curium values from rare earth values. In accordance with the invention americium, curium, and rare earth values are sorbed on an anion exchange resin. A major portion of the rare earth values are selectively stripped from the resin with a concentrated aqueous solution of lithium chloride, and americium, curium, and a minor portion of rare earth values are then stripped from the resin with a dilute aqueous solution of lithium chloride. The americium and curium values are further purified by increasing the concentration of lithium chloride in the solution to at least 8 molar and selectively extracting rare earth values from the resulting solution with a monoalkylphosphoric acid. (AEC)

  18. Plutonium and Americium Geochemistry at Hanford: A Site Wide Review

    SciTech Connect

    Cantrell, Kirk J.; Felmy, Andrew R.

    2012-08-23

    This report was produced to provide a systematic review of the state-of-knowledge of plutonium and americium geochemistry at the Hanford Site. The report integrates existing knowledge of the subsurface migration behavior of plutonium and americium at the Hanford Site with available information in the scientific literature regarding the geochemistry of plutonium and americium in systems that are environmentally relevant to the Hanford Site. As a part of the report, key research needs are identified and prioritized, with the ultimate goal of developing a science-based capability to quantitatively assess risk at sites contaminated with plutonium and americium at the Hanford Site and the impact of remediation technologies and closure strategies.

  19. Americium/Curium Disposition Life Cycle Planning Study

    SciTech Connect

    Jackson, W.N.; Krupa, J.; Stutts, P.; Nester, S.; Raimesch, R.

    1998-04-30

    At the request of the Department of Energy Savannah River Office (DOE- SR), Westinghouse Savannah River Company (WSRC) evaluated concepts to complete disposition of Americium and Curium (Am/Cm) bearing materials currently located at the Savannah River Site (SRS).

  20. Tributylphosphate Extraction Behavior of Bismuthate-Oxidized Americium

    SciTech Connect

    Mincher; Leigh R. Martin; Nicholas C. Schmitt

    2008-08-01

    Higher oxidation states of americium have long been known; however, options for their preparation in acidic solution are limited. The conventional choice, silver-catalyzed peroxydisulfate, is not useful at nitric acid concentrations above about 0.3 M. We investigated the use of sodium bismuthate as an oxidant for Am3+ in acidic solution. Room-temperature oxidation produced AmO2 2+ quantitatively, whereas oxidation at 80 °C produced AmO2+ quantitatively. The efficacy of the method for the production of oxidized americium was verified by fluoride precipitation and by spectroscopic absorbance measurements. We performed absorbance measurements using a conventional 1 cm cell for high americium concentrations and a 100 cm liquid waveguide capillary cell for low americium concentrations. Extinction coefficients for the absorbance of Am3+ at 503 nm, AmO2+ at 514 nm, and AmO2 2+ at 666 nm in 0.1 M nitric acid are reported. We also performed solvent extraction experiments with the hexavalent americium using the common actinide extraction ligand tributyl phosphate (TBP) for comparison to the other hexavalent actinides. Contact with 30% tributyl phosphate in dodecane reduced americium; it was nevertheless extracted using short contact times. The TBP extraction of AmO2 2+ over a range of nitric acid concentrations is shown for the first time and was found to be analogous to that of uranyl, neptunyl, and plutonyl ions.

  1. Discovery of isotopes of the transuranium elements with 93≤Z≤98

    SciTech Connect

    Fry, C.; Thoennessen, M.

    2013-01-15

    One hundred and five isotopes of the transuranium elements neptunium, plutonium, americium, curium, berkelium, and californium have been observed so far; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  2. Discovery of isotopes of the transuranium elements with 93≤Z≤98

    NASA Astrophysics Data System (ADS)

    Fry, C.; Thoennessen, M.

    2013-01-01

    One hundred and five isotopes of the transuranium elements neptunium, plutonium, americium, curium, berkelium, and californium have been observed so far; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  3. Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides

    NASA Astrophysics Data System (ADS)

    Horlait, Denis; Caraballo, Richard; Lebreton, Florent; Jégou, Christophe; Roussel, Pascal; Delahaye, Thibaud

    2014-09-01

    Americium oxides samples were characterized by X-ray diffraction (XRD) and Raman spectroscopy, with an emphasis on their structural behavior under oxidation and self-irradiation. Raman spectra of americium dioxide (AmO2) and sesquioxide (Am2O3) were obtained for the first time. With the help of literature data on isostructural oxides, Raman signatures of Ia-3 C-type Am2O3 and P-3m1 A-type Am2O3 are identified. For AmO2, a clear band is noted at 390 cm-1. Its nature is compared to that of the other actinide dioxides. Am2O3 evolution under ambient conditions and against 241Am α self-irradiation was monitored by powder XRD. The sample, initially composed of A-type Am2O3 as major phase as well as C2/m B-type and C-type structures as minor phases, progressively oxidizes to Fm-3m AmO2-δ over a few months. On the basis of diffractogram refinements, evolutions of unit cell volumes caused by self-irradiation are also determined and discussed.

  4. RCRA designation of discarded americium/beryllium sealed sources

    SciTech Connect

    Kirner, N.P.

    1994-09-01

    Many sealed sources containing americium and beryllium are used throughout construction, industry, and research, and will eventually require disposal. For planning purposes it is necessary to determine whether these sources, when disposed, constitute a mixed waste, i.e., a waste containing hazardous constituents regulated under the Resource Conservation and Recovery Act and radioactive constituents regulated under the Atomic Energy Act. Waste designation criteria contained in 40 CFR 261 are evaluated in detail in this report. It is determined that discarded americium/beryllium sealed sources do not contain any wastes listed in Subpart D of 40 CFR 261, nor do the discarded sources exhibit any hazardous characteristics. Therefore, it is concluded that discarded americium/beryllium sealed sources are not a mixed waste under regulations established by the US Environmental Protection Agency. Hazardous waste regulatory programs delegated to States, however, may have regulations that differ from those of the Federal government.

  5. A TRUEX-based separation of americium from the lanthanides

    SciTech Connect

    Bruce J. Mincher; Nicholas C. Schmitt; Mary E. Case

    2011-03-01

    Abstract: The inextractability of the actinide AnO2+ ions in the TRUEX process suggests the possibility of a separation of americium from the lanthanides using oxidation to Am(V). The only current method for the direct oxidation of americium to Am(V) in strongly acidic media is with sodium bismuthate. We prepared Am(V) over a wide range of nitric acid concentrations and investigated its solvent extraction behavior for comparison to europium. While a separation is achievable in principal, the presence of macro amounts of cerium competes for the sparingly soluble oxidant and the oxidant itself competes for CMPO complexation. These factors conspire to reduce the Eu/Am separation factor from ~40 using tracer solutions to ~5 for extractions from first cycle raffinate simulant solution. To separate pentavalent americium directly from the lanthanides using the TRUEX process, an alternative oxidizing agent will be necessary.

  6. Experimental Measurements of Short-Lived Fission Products from Uranium, Neptunium, Plutonium and Americium

    SciTech Connect

    Metz, Lori A.; Payne, Rosara F.; Friese, Judah I.; Greenwood, Lawrence R.; Kephart, Jeremy D.; Pierson, Bruce D.

    2009-11-01

    Fission yields are especially well characterized for long-lived fission products. Modeling techniques incorporate numerous assumptions and can be used to deduce information about the distribution of short-lived fission products. This work is an attempt to gather experimental (model-independent) data on the short-lived fission products. Fissile isotopes of uranium, neptunium, plutonium and americium were irradiated under pulse conditions at the Washington State University 1 MW TRIGA reactor to achieve ~108 fissions. The samples were placed on a HPGe (high purity germanium) detector to begin counting in less than 3 minutes post irradiation. The samples were counted for various time intervals ranging from 5 minutes to 1 hour. The data was then analyzed to determine which radionuclides could be quantified and compared to the published fission yield data.

  7. Low energy AMS of americium and curium

    NASA Astrophysics Data System (ADS)

    Christl, Marcus; Dai, Xiongxin; Lachner, Johannes; Kramer-Tremblay, Sheila; Synal, Hans-Arno

    2014-07-01

    Accelerator mass spectrometry (AMS) has evolved over the past years as one of the most sensitive, selective, and robust techniques for actinide analyses. While analyses of U and Pu isotopes have already become routine at the ETH Zurich 0.5 MV AMS system "Tandy", there is an increasing demand for highly sensitive analyses of the higher actinides such as Am and Cm for bioassay applications and beyond. In order to extend the actinide capabilities of the compact ETH Zurich AMS system and to develop new, more sensitive bioassay routines, a pilot study was carried out. The aim was to investigate and document the performance and the potential background of Am and Cm analyses with low energy AMS. Our results show that 241Am and Cm isotopes can be determined relative to a 243Am tracer if samples and AMS standards are prepared identically with regard to the matrix elements, in which the sample is dispersed. In this first test, detection limits for Cm and Am isotopes are all in the sub-femtogram range and even below 100 ag for Cm isotopes. In a systematic background study in the mass range of the Cm isotopes, two formerly unknown metastable triply charged Th molecules were found on amu(244) and amu(248). The presence of such a background is not a principal problem for AMS if the stripper pressure is increased accordingly. Based on our first results, we conclude that ultra-trace analyses of Am and Cm isotopes for bioassay are very well possible with low energy AMS.

  8. PLUTONIUM-239 AND AMERICIUM-241 UPTAKE BY PLANTS FROM SOIL

    EPA Science Inventory

    Alfalfa was grown in soil contaminated with plutonium-239 dioxide (239PuO2) at a concentration of 29.7 nanocuries per gram (nCi/g). In addition to alfalfa, radishes, wheat, rye, and tomatoes were grown in soils contaminated with americium-241 nitrate (241Am(NO3)3) at a concentrat...

  9. SIMULTANEOUS DETERMINATION OF AMERICIUM AND CURIUM IN SOIL

    EPA Science Inventory

    A method is presented for the routine determination of americium and curium in 10 g of soil. The soil is dissolved with a mixture of nitric acid and hydrofluoric acid. Insoluble sulfates and phosphates are metathesized with boiling sodium hydroxide solutions. Plutonium and iron a...

  10. Supercritical Fluid Extraction of Plutonium and Americium from Soil

    SciTech Connect

    Fox, R.V.; Mincher, B.J.

    2002-05-23

    Supercritical fluid extraction (SFE) of plutonium and americium from soil was successfully demonstrated using supercritical fluid carbon dioxide solvent augmented with organophosphorus and beta-diketone complexants. Spiked Idaho soils were chemically and radiologically characterized, then extracted with supercritical fluid carbon dioxide at 2,900 psi and 65 C containing varying concentrations of tributyl phosphate (TBP) and thenoyltrifluoroacetone (TTA). A single 45 minute SFE with 2.7 mol% TBP and 3.2 mol% TTA provided as much as 88% {+-} 6.0 extraction of americium and 69% {+-} 5.0 extraction of plutonium. Use of 5.3 mol% TBP with 6.8 mol% of the more acidic beta-diketone hexafluoroacetylacetone (HFA) provided 95% {+-} 3.0 extraction of americium and 83% {+-} 5.0 extraction of plutonium in a single 45 minute SFE at 3,750 psi and 95 C. Sequential chemical extraction techniques were used to chemically characterize soil partitioning of plutonium and americium in pre-SFE soil samples. Sequential chemical extraction techniques demonstrated that spiked plutonium resides primarily (76.6%) in the sesquioxide fraction with minor amounts being absorbed by the oxidizable fraction (10.6%) and residual fractions (12.8%). Post-SFE soils subjected to sequential chemical extraction characterization demonstrated that 97% of the oxidizable, 78% of the sesquioxide and 80% of the residual plutonium could be removed using SFE. These preliminary results show that SFE may be an effective solvent extraction technique for removal of actinide contaminants from soil.

  11. Reduction Rates for Higher Americium Oxidation States in Nitric Acid

    SciTech Connect

    Grimes, Travis Shane; Mincher, Bruce Jay; Schmitt, Nicholas C

    2015-09-30

    The stability of hexavalent americium was measured using multiple americium concentrations and nitric acid concentrations after contact with the strong oxidant sodium bismuthate. Contrary to our hypotheses Am(VI) was not reduced faster at higher americium concentrations, and the reduction was only zero-order at short time scales. Attempts to model the reduction kinetics using zero order kinetic models showed Am(VI) reduction in nitric acid is more complex than the autoreduction processes reported by others in perchloric acid. The classical zero-order reduction of Am(VI) was found here only for short times on the order of a few hours. We did show that the rate of Am(V) production was less than the rate of Am(VI) reduction, indicating that some Am(VI) undergoes two electron-reduction to Am(IV). We also monitored the Am(VI) reduction in contact with the organic diluent dodecane. A direct comparison of these results with those in the absence of the organic diluent showed the reduction rates for Am(VI) were not statistically different for both systems. Additional americium oxidations conducted in the presence of Ce(IV)/Ce(III) ions showed that Am(VI) is reduced without the typical growth of Am(V) observed in the systems sans Ce ion. This was an interesting result which suggests a potential new reduction/oxidation pathway for Am in the presence of Ce; however, these results were very preliminary, and will require additional experiments to understand the mechanism by which this occurs. Overall, these studies have shown that hexavalent americium is fundamentally stable enough in nitric acid to run a separations process. However, the complicated nature of the reduction pathways based on the system components is far from being rigorously understood.

  12. Ingestion Pathway Transfer Factors for Plutonium and Americium

    SciTech Connect

    Blanchard, A.

    1999-07-28

    Overall transfer factors for major ingestion pathways are derived for plutonium and americium. These transfer factors relate the radionuclide concentration in a given foodstuff to deposition on the soil. Equations describing basic relationships consistent with Regulatory Guide 1.109 are followed. Updated values and coefficients from IAEA Technical Reports Series No. 364 are used when a available. Preference is given to using factors specific to the Savannah River Site.

  13. Supercritical Fluid Extraction of Plutonium and Americium from Soil

    SciTech Connect

    Fox, Robert Vincent; Mincher, Bruce Jay

    2002-08-01

    Supercritical fluid extraction (SFE) of plutonium and americium from soil was successfully demonstrated using supercritical fluid carbon dioxide solvent augmented with organophosphorus and beta-diketone complexants. Spiked Idaho soils were chemically and radiologically characterized, then extracted with supercritical fluid carbon dioxide at 2,900 psi and 65°C containing varying concentrations of tributyl phosphate (TBP) and thenoyltrifluoroacetone (TTA). A single 45 minute SFE with 2.7 mol% TBP and 3.2 mol% TTA provided as much as 88% ± 6.0 extraction of americium and 69% ± 5.0 extraction of plutonium. Use of 5.3 mol% TBP with 6.8 mol% of the more acidic beta-diketone hexafluoroacetylacetone (HFA) provided 95% ± 3.0 extraction of americium and 83% ± 5.0 extraction of plutonium in a single 45 minute SFE at 3,750 psi and 95°C. Sequential chemical extraction techniques were used to chemically characterize soil partitioning of plutonium and americium in pre-SFE soil samples. Sequential chemical extraction techniques demonstrated that spiked plutonium resides primarily (76.6%) in the sesquioxide fraction with minor amounts being absorbed by the oxidizable fraction (10.6%) and residual fractions (12.8%). Post-SFE soils subjected to sequential chemical extraction characterization demonstrated that 97% of the oxidizable, 78% of the sesquioxide and 80% of the residual plutonium could be removed using SFE. These preliminary results show that SFE may be an effective solvent extraction technique for removal of actinide contaminants from soil.

  14. Method for removal of plutonium impurity from americium oxides and fluorides

    DOEpatents

    FitzPatrick, John R.; Dunn, Jerry G.; Avens, Larry R.

    1987-01-01

    Method for removal of plutonium impurity from americium oxides and fluorides. AmF.sub.4 is not further oxidized to AmF.sub.6 by the application of O.sub.2 F at room temperature, while plutonium compounds present in the americium sample are fluorinated to volatile PuF.sub.6, which can readily be separated therefrom, leaving the purified americium oxides and/or fluorides as the solid tetrafluoride.

  15. Method for removal of plutonium impurity from americium oxides and fluorides

    DOEpatents

    FitzPatrick, J.R.; Dunn, J.G.; Avens, L.R.

    1987-02-13

    Method for removal of plutonium impurity from americium oxides and fluorides. AmF/sub 4/ is not further oxidized to AmF/sub 6/ by the application of O/sub 2/F at room temperature thereto, while plutonium compounds present in the americium sample are fluorinated to volatile PuF/sub 6/, which can readily be separated therefrom, leaving the purified americium oxides and/or fluorides as the solid tetrafluoride thereof.

  16. AMERICIUM SEPARATIONS FROM NITRIC ACID PROCESS EFFLUENT STREAMS

    SciTech Connect

    M. BARR; G. JARVINEN; ET AL

    2000-08-01

    The aging of the US nuclear stockpile presents a number of challenges, including the ever-increasing radioactivity of plutonium residues from {sup 241}Am. Minimization of this weak gamma-emitter in process and waste solutions is desirable to reduce both worker exposure and the effects of radiolysis on the final waste product. Removal of americium from plutonium nitric acid processing effluents, however, is complicated by the presence of large.quantities of competing metals, particularly Fe and Al, and-strongly oxidizing acidic solutions. The reprocessing operation offers several points at which americium removal maybe attempted, and we are evaluating two classes of materials targeted at different steps in the process. Extraction chromatography resin materials loaded with three different alkylcarbamoyl phosphinates and phosphine oxides were accessed for Am removal efficiency and Am/Fe selectivity from 1-7 molar nitric acid solutions. Commercial and experimental mono- and bifunctional anion-exchange resins were evaluated for total alpha-activity removal from post-evaporator solutions whose composition, relative to the original nitric acid effluent, is reduced in acid and greatly increased in total salt content. With both classes of materials, americium/total alpha emission removal is sufficient to meet regulatory requirements even under sub-optimal conditions. Batch distribution coefficients, column performance data, and the effects of Fe-masking agents will be presented.

  17. Neptunium and americium speciation in selected basalt, granite, shale, and tuff ground waters

    USGS Publications Warehouse

    Cleveland, J.M.; Rees, T.F.; Nash, K.L.

    1983-01-01

    Neptunium and americium are relatively insoluble in ground waters containing high sulfate concentrations, particularly at 90??C. The insoluble neptunium species is Np(IV); hence reducing waters should enhance its formation. Americium can exist only in the trivalent state under these conditions, and its solubility also should be representative of that of curium.

  18. 10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... 10 Energy 1 2012-01-01 2012-01-01 false Calibration or reference sources containing americium-241... americium-241 or radium-226: Requirements for license to manufacture or initially transfer. An application... containing americium-241 or radium-226, for distribution to persons generally licensed under § 31.8 of...

  19. 10 CFR 32.102 - Schedule C-prototype tests for calibration or reference sources containing americium-241 or...

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... sources containing americium-241 or radium-226. 32.102 Section 32.102 Energy NUCLEAR REGULATORY COMMISSION... americium-241 or radium-226. An applicant for a license under § 32.57 shall, for any type of source which is designed to contain more than 0.185 kilobecquerel (0.005 microcurie) of americium-241 or...

  20. 10 CFR 32.102 - Schedule C-prototype tests for calibration or reference sources containing americium-241 or...

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... sources containing americium-241 or radium-226. 32.102 Section 32.102 Energy NUCLEAR REGULATORY COMMISSION... americium-241 or radium-226. An applicant for a license under § 32.57 shall, for any type of source which is designed to contain more than 0.185 kilobecquerel (0.005 microcurie) of americium-241 or...

  1. 10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... 10 Energy 1 2010-01-01 2010-01-01 false Calibration or reference sources containing americium-241... americium-241 or radium-226: Requirements for license to manufacture or initially transfer. An application... containing americium-241 or radium-226, for distribution to persons generally licensed under § 31.8 of...

  2. 10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... 10 Energy 1 2014-01-01 2014-01-01 false Calibration or reference sources containing americium-241... americium-241 or radium-226: Requirements for license to manufacture or initially transfer. An application... containing americium-241 or radium-226, for distribution to persons generally licensed under § 31.8 of...

  3. 10 CFR 31.8 - Americium-241 and radium-226 in the form of calibration or reference sources.

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... 10 Energy 1 2014-01-01 2014-01-01 false Americium-241 and radium-226 in the form of calibration or... BYPRODUCT MATERIAL § 31.8 Americium-241 and radium-226 in the form of calibration or reference sources. (a..., americium-241 or radium-226 in the form of calibration or reference sources: (1) Any person in a...

  4. 10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

    Code of Federal Regulations, 2013 CFR

    2013-01-01

    ... 10 Energy 1 2013-01-01 2013-01-01 false Calibration or reference sources containing americium-241... americium-241 or radium-226: Requirements for license to manufacture or initially transfer. An application... containing americium-241 or radium-226, for distribution to persons generally licensed under § 31.8 of...

  5. 10 CFR 32.57 - Calibration or reference sources containing americium-241 or radium-226: Requirements for license...

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... 10 Energy 1 2011-01-01 2011-01-01 false Calibration or reference sources containing americium-241... americium-241 or radium-226: Requirements for license to manufacture or initially transfer. An application... containing americium-241 or radium-226, for distribution to persons generally licensed under § 31.8 of...

  6. 10 CFR 32.102 - Schedule C-prototype tests for calibration or reference sources containing americium-241 or...

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... sources containing americium-241 or radium-226. 32.102 Section 32.102 Energy NUCLEAR REGULATORY COMMISSION... americium-241 or radium-226. An applicant for a license under § 32.57 shall, for any type of source which is designed to contain more than 0.185 kilobecquerel (0.005 microcurie) of americium-241 or...

  7. High pressure phase transition and elastic properties of americium telluride

    NASA Astrophysics Data System (ADS)

    Aynyas, Mahendra; Rukmangad, Aditi; Arya, B. S.; Sanyal, S. P.

    2013-06-01

    The structural and elastic properties of Americium Telluride (AmTe) have been investigated by using a modified inter-ionic potential theory (MIPT). This theory is capable of explaining first order phase transition with a crystallographic change NaCl to CsCl structure for this compound. The values of optimized lattice constant, phase transition pressure, zero pressure bulk modulus and second order elastic constants (C11, C44) agree well with their corresponding experimental data. Debye temperature (θD) is also calculated for this compound for the first time.

  8. Passive field monitoring of plutonium and americium in soil

    SciTech Connect

    Gammage, R.B.; Meyer, K.E.; Dudney, C.S.

    1994-12-31

    The authors` progress is described in applying passive alpha track detectors (ATDS) and electret ion chambers (EICS) to in-situ field monitoring of soils contaminated with particulate plutonium and americium at a desert site. By varying the exposure times, from a few minutes to about one day, they quantitatively measured alpha activity varying between {approximately} 100 pCi/g and {approximately} 100 nCi/g. Suggested applications are definition of the boundaries of contamination zones and verification that post-remediated soils are below release limits.

  9. Quantitative NDA measurements of advanced reprocessing product materials containing uranium, neptunium, plutonium, and americium

    NASA Astrophysics Data System (ADS)

    Goddard, Braden

    The ability of inspection agencies and facility operators to measure powders containing several actinides is increasingly necessary as new reprocessing techniques and fuel forms are being developed. These powders are difficult to measure with nondestructive assay (NDA) techniques because neutrons emitted from induced and spontaneous fission of different nuclides are very similar. A neutron multiplicity technique based on first principle methods was developed to measure these powders by exploiting isotope-specific nuclear properties, such as the energy-dependent fission cross sections and the neutron induced fission neutron multiplicity. This technique was tested through extensive simulations using the Monte Carlo N-Particle eXtended (MCNPX) code and by one measurement campaign using the Active Well Coincidence Counter (AWCC) and two measurement campaigns using the Epithermal Neutron Multiplicity Counter (ENMC) with various (alpha,n) sources and actinide materials. Four potential applications of this first principle technique have been identified: (1) quantitative measurement of uranium, neptunium, plutonium, and americium materials; (2) quantitative measurement of mixed oxide (MOX) materials; (3) quantitative measurement of uranium materials; and (4) weapons verification in arms control agreements. This technique still has several challenges which need to be overcome, the largest of these being the challenge of having high-precision active and passive measurements to produce results with acceptably small uncertainties.

  10. Comparative biokinetics of trivalent radionuclides with similar ionic dimensions: promethium-147, curium-242 and americium-241.

    PubMed

    Priest, N D

    2007-09-01

    Data on the distribution and redistribution patterns in the laboratory rat of three trivalent elements with a similar ionic radius have been compared. This showed that these distributions for the two ions with the same ionic radius (111 pm), i.e., those of promethium (a lanthanoid) and curium (an actinoid), were indistinguishable and that americium, with a slightly larger ion size (111.5 pm), behaved similarly. The results are consistent with the suggestion that ion size is the only important factor controlling the deposition and redistribution patterns of trivalent lanthanoids and actinoids in rats. The result is important because it suggests that the same radiological protection dosimetry models should be used for trivalent actinoids and lanthanoids, that human volunteer data generated for lanthanoid isotopes can be used to predict the behavior of actinoids with the same ion size, and that appropriate pairs of beta-particle-emitting lanthanoid and alpha-particle-emitting actinoids could be used to study the relative toxicity of alpha and beta particles in experimental animals. PMID:17705633

  11. A Density Functional Study of the Americium (001) Surface

    NASA Astrophysics Data System (ADS)

    Gao, Da; Ray, Asok Kumar

    2006-03-01

    Electronic structure properties of the fcc americium (001) surface, modeled by periodically repeated fcc Am (001) surface slabs, have been studied with the full-potential linearized augmented plane wave (FP-LAPW) method. The alternative basis set APW+lo is used inside the atomic spheres for chemically important orbitals that are difficult to converge, whereas LAPW is used for others. The core states are treated fully relativistically and for valence states, two levels of treatments are implemented: (1) a scalar relativistic scheme including the mass-velocity correction and the Darwin s-shift and (2) a fully relativistic scheme with spin-orbit coupling included in a second variational treatment using the scalar-relativistic eigenfunctions as basis. Our results indicate that the ground state of Am (001) surface is anti-ferromagnetic. The quantum size effects in the surface energies and the work functions of the (001) fcc americium ultra thin films (UTF) have been examined up to seven layers. In addition, the Am (001) surface properties are compared with our earlier study of the Am (111) surface.

  12. Americium Transmutation Feasibility When Used as Burnable Absorbers - 12392

    SciTech Connect

    Barbaras, Sean A.; Knight, Travis W.

    2012-07-01

    The use of plutonium in Mixed Oxide (MOX) fuel in traditional Pressurized Water Reactor (PWR) assemblies leads to greater americium production which is not addressed in MOX recycling. The transuranic nuclides (TRU) contribute the most to the radiotoxicity of nuclear waste and a reduction of the TRU stockpile would greatly reduce the overall radiotoxicity of what must be managed. Am-241 is a TRU of particular concern because it is the dominant contributor of total radiotoxicity for the first 1000 years in a repository. This research explored the feasibility of transmuting Am-241 by using varying amounts in MOX rods being used in place of burnable absorbers and evaluated with respect to the impact on incineration and transmutation of transuranics in MOX fuel as well as the impact on safety. This research concludes that the addition of americium to a non-uniform fuel assembly is a viable method of transmuting Am-241, holding down excess reactivity in the core while serving as a burnable poison, as well as reducing the radiotoxicity of high level waste that must be managed. The use of Am/MOX hybrid fuel assemblies to transmute americium was researched using multiple computer codes. Am-241 was shown in this study to be able to hold down excess reactivity at the beginning of cycle and shape the power distribution in the core with assemblies of varying americium content loaded in a pattern similar to the traditional use of assemblies with varying amounts of burnable absorbers. The feasibility, safety, and utility of using americium to create an Am/MOX hybrid non-uniform core were also evaluated. The core remained critical to a burnup of 22,000 MWD/MTM. The power coefficient of reactivity as well as the temperature and power defects were sufficiently negative to provide a prompt feedback mechanism in case of a transient and prevent a power excursion, thus ensuring inherent safety and protection of the core. As shown here as well as many other studies, this non

  13. Extraction of americium in different oxidation states in a two-phase aqueous system based on poly(ethylene glycol)

    SciTech Connect

    Molochnikova, N.P.; Frenkel', B.F.; Myasoedov, B.F.; Shkinev, V.M.; Spivakov, B.Ya.; Zolotov, Yu.A.

    1987-09-01

    The extraction of americium in different states of oxidation was studied in a two-phase aqueous system based on poly(ethylene glycol). Conditions were found for the quantitative extraction of americium (III) and americium (V) from solutions of ammonium sulfate in the pH range of 3-5 and in the presence of arsenazo III. The composition of the complexes of americium with the reagent was determined; americium (III) reacts with arsenazo III in solutions of ammonium sulfate to form complexes with the composition of MeR and Me/sub 2/R. Characteristics of the absorption spectra of complexes of americium (III) and (V) with arsenazo III in ammonium sulfate solutions and in extracts based on aqueous solutions of poly(ethylene glycol) were found. The molar extinction coefficients of complexes of americium with arsenazo III were determined in these solutions.

  14. The 1976 Hanford Americium Accident: Then and Now

    SciTech Connect

    Carbaugh, Eugene H.

    2013-10-02

    The 1976 chemical explosion of an 241Am ion exchange column at a Hanford Site waste management facility resulted in the extreme contamination of a worker with 241Am, nitric acid and debris. The worker underwent medical treatment for acid burns, as well as wound debridement, extensive personal skin decontamination and long-term DTPA chelation therapy for decorporation of americium-241. Because of the contamination levels and prolonged decontamination efforts, care was provided for the first three months at the unique Emergency Decontamination Facility with gradual transition to the patient’s home occurring over another two months. The medical treatment, management, and dosimetry of the patient have been well documented in numerous reports and journal articles. The lessons learned with regard to patient treatment and effectiveness of therapy still form the underlying philosophy of treatment for contaminated injuries. Changes in infrastructure and facilities as well as societal expectations make for interesting speculation as to how responses might differ today.

  15. Separation of americium from curium by oxidation and ion exchange.

    PubMed

    Burns, Jonathan D; Shehee, Thomas C; Clearfield, Abraham; Hobbs, David T

    2012-08-21

    Nuclear energy has the potential to be a clean alternative to fossil fuels, but in order for it to play a major role in the US, many questions about the back end of the fuel cycle must be addressed. One of these questions is the difficult separation of americium from curium. Here, we report the oxidation of Am in two systems, perchloric acid and nitric acid and the affect of changing the acid has on the oxidation. K(d) values were observed and a direct separation factor was calculated and was seen to be as high as 20 for four metal(IV) pillared phosphate phosphonate inorganic organic hybrid ion exchange materials. These ion exchangers are characterized by very low selectivity for cations with low charge but extremely high uptake of ions of high charge. PMID:22827724

  16. Monte Carlo modeling of spallation targets containing uranium and americium

    NASA Astrophysics Data System (ADS)

    Malyshkin, Yury; Pshenichnov, Igor; Mishustin, Igor; Greiner, Walter

    2014-09-01

    Neutron production and transport in spallation targets made of uranium and americium are studied with a Geant4-based code MCADS (Monte Carlo model for Accelerator Driven Systems). A good agreement of MCADS results with experimental data on neutron- and proton-induced reactions on 241Am and 243Am nuclei allows to use this model for simulations with extended Am targets. It was demonstrated that MCADS model can be used for calculating the values of critical mass for 233,235U, 237Np, 239Pu and 241Am. Several geometry options and material compositions (U, U + Am, Am, Am2O3) are considered for spallation targets to be used in Accelerator Driven Systems. All considered options operate as deep subcritical targets having neutron multiplication factor of k∼0.5. It is found that more than 4 kg of Am can be burned in one spallation target during the first year of operation.

  17. Plutonium, americium, and neptunium speciation in selected groundwaters

    USGS Publications Warehouse

    Cleveland, J.M.; Rees, T.F.; Nash, K.L.

    1985-01-01

    Speciation was determined at 25 and 90 degree C in four groundwaters from diverse sources: the Sparta aquifer in Louisiana, near the Vacherie salt dome; Mansfield No. 2 well in the Palo Duro Basin, Texas; the Stripa mine in Sweden; and the Waste Isolation Pilot Plant in New Mexico. Neptunium generally was soluble in all waters and was present exclusively as Np(V) and Np(VI), regardless of initial oxidation state. The results indicated that plutonium and neptunium solubilities were determined by the oxidation-reduction properties of the waters, i. e. , their abilities to convert these elements to soluble oxidation states. This was not the case for americium, however; Am(IV) was not detected, and the solubility of this element was determined entirely by the chemical properties of Am(III).

  18. 1976 Hanford americium exposure incident: in vivo measurements

    SciTech Connect

    Palmer, H.E.; Rieksts, G.A.; Icayan, E.E.

    1982-01-01

    Detailed external measurement were made of internally deposited /sup 241/Am in a nuclear chemical operator involved in an americium exposure accident at the Hanford plant. Despite some interference from high-level external contamination, quantitative measurements of the /sup 241/Am content in the lung, liver, and bones were made starting on the third day after the accident. The rate of excretion of /sup 241/Am from these organs was determined. The /sup 241/Am embedded in the skin of the face and head was carefully mapped. The distribution over the total length of the body was also determined. Linear and rectilinear scanners, gamma cameras, large and small scintillation detectors, proportional counters, and Si(Li) and intrinsic germanium detectors were used to evaluate the internal deposition. Methods of calibration for quantitative measurement included simulation of the /sup 241/Am activity in both phantom and cadaver parts.

  19. Relativistic density functional theory modeling of plutonium and americium higher oxide molecules.

    PubMed

    Zaitsevskii, Andréi; Mosyagin, Nikolai S; Titov, Anatoly V; Kiselev, Yuri M

    2013-07-21

    The results of electronic structure modeling of plutonium and americium higher oxide molecules (actinide oxidation states VI through VIII) by two-component relativistic density functional theory are presented. Ground-state equilibrium molecular structures, main features of charge distributions, and energetics of AnO3, AnO4, An2On (An=Pu, Am), and PuAmOn, n = 6-8, are determined. In all cases, molecular geometries of americium and mixed plutonium-americium oxides are similar to those of the corresponding plutonium compounds, though chemical bonding in americium oxides is markedly weaker. Relatively high stability of the mixed heptoxide PuAmO7 is noticed; the Pu(VIII) and especially Am(VIII) oxides are expected to be unstable. PMID:23883027

  20. Relativistic density functional theory modeling of plutonium and americium higher oxide molecules

    NASA Astrophysics Data System (ADS)

    Zaitsevskii, Andréi; Mosyagin, Nikolai S.; Titov, Anatoly V.; Kiselev, Yuri M.

    2013-07-01

    The results of electronic structure modeling of plutonium and americium higher oxide molecules (actinide oxidation states VI through VIII) by two-component relativistic density functional theory are presented. Ground-state equilibrium molecular structures, main features of charge distributions, and energetics of AnO3, AnO4, An2On (An=Pu, Am), and PuAmOn, n = 6-8, are determined. In all cases, molecular geometries of americium and mixed plutonium-americium oxides are similar to those of the corresponding plutonium compounds, though chemical bonding in americium oxides is markedly weaker. Relatively high stability of the mixed heptoxide PuAmO7 is noticed; the Pu(VIII) and especially Am(VIII) oxides are expected to be unstable.

  1. Oxidative Alkaline leaching of Americium from simulated high-level nuclear waste sludges

    SciTech Connect

    Reed, Wendy A.; Garnov, Alexander Yu.; Rao, Linfeng; Nash, Kenneth L.; Bond, Andrew H.

    2004-01-23

    Oxidative alkaline leaching has been proposed to pre-treat the high-level nuclear waste sludges to remove some of the problematic (e.g., Cr) and/or non-radioactive (e.g., Na, Al) constituents before vitrification. It is critical to understand the behavior of actinides, americium and plutonium in particular, in oxidative alkaline leaching. We have studied the leaching behavior of americium from four different sludge simulants (BiPO{sub 4}, BiPO{sub 4 modified}, Redox, PUREX) using potassium permanganate and potassium persulfate in alkaline solutions. Up to 60% of americium sorbed onto the simulants is leached from the sludges by alkaline persulfate and permanganate. The percentage of americium leached increases with [NaOH] (between 1.0 and 5.0 M). The initial rate of americium leaching by potassium persulfate increases in the order BiPO{sub 4} sludge < Redox sludge < PUREX sludge. The data are most consistent with oxidation of Am{sup 3+} in the sludge to either AmO{sub 2}{sup +} or AmO{sub 2}{sup 2+} in solution. Though neither of these species is expected to exhibit long-term stability in solution, the potential for mobilization of americium from sludge samples would have to be accommodated in the design of any oxidative leaching process for real sludge samples.

  2. Characterization of a Sealed Americium-Beryllium (AmBe) Source by Inductively Coupled Plasma Mass Spectrometry

    SciTech Connect

    James Sommers; Marcos Jimenez; Mary Adamic; Jeffrey Giglio; Kevin Carney

    2009-12-01

    Two Americium-Beryllium neutron sources were dismantled, sampled (sub-sampled) and analyzed via inductively coupled plasma mass spectrometry (ICP-MS). Characteristics such as “age” since purification, actinide content, trace metal content and inter and intra source composition were determined. The “age” since purification of the two sources was determined to be 25.0 and 25.4 years, respectively. The systematic errors in the “age” determination were ± 4 % 2s. The amount and isotopic composition of U and Pu varied substantially between the sub-samples of Source 2 (n=8). This may be due to the physical means of sub-sampling or the way the source was manufactured. Source 1 was much more consistent in terms of content and isotopic composition (n=3 sub-samples). The Be-Am ratio varied greatly between the two sources. Source 1 had an Am-Be ratio of 6.3 ± 52 % (1s). Source 2 had an Am-Be ratio of 9.81 ± 3.5 % (1s). In addition, the trace element content between the samples varied greatly. Significant differences were determined between Source 1 and 2 for Sc, Sr, Y, Zr, Mo, Ba and W.

  3. Electronic, mechanical, and thermodynamic properties of americium dioxide

    NASA Astrophysics Data System (ADS)

    Lu, Yong; Yang, Yu; Zheng, Fawei; Wang, Bao-Tian; Zhang, Ping

    2013-10-01

    By performing density functional theory (DFT) +U calculations, we systematically study the electronic, mechanical, tensile, and thermodynamic properties of AmO2. It is found that the chemical bonding character in AmO2 is similar to that in PuO2, with smaller charge transfer and stronger covalent interactions between americium and oxygen atoms. The stress-strain relationship of AmO2 is examined along the three low-index directions, showing that the [1 0 0] and [1 1 1] directions are the strongest and weakest tensile directions, respectively, but the theoretical tensile strengths of AmO2 are smaller than those of PuO2. The phonon dispersion curves of AmO2 are calculated and the heat capacities as well as lattice expansion curve are subsequently determined. The lattice thermal conductivity of AmO2 is further evaluated and compared with attainable experiments. Our present work integrally reveals various physical properties of AmO2 and can be referenced for technological applications of AmO2 based materials.

  4. Environmental impact of a teratogenic actinide: a case study of americium-241

    SciTech Connect

    Wang, J.; Yang, J.Y.

    1985-10-16

    Americium-241 is widely used as a radiation source, but it also has some potential risk if taken into the body. Although the radiotoxicity of americium-241 is small compared to other transuranic actinides, its effects on the reproductive system and on development of the placenta are more damaging than the effects of plutonium-239. A previous report based on a worst-case scenario involving a hypothetical fire accident in a contaminated facility indicated that there could have been a significant impact on nearby residents from a unit release of americium-241 via atmospheric dispersion. However, because the facility is located in a rural region where most drinking water supplies are drawn from private wells, it is believed that deposition of americium-241 from the atmosphere might also have impacts via the groundwater pathway by infiltration of rainwater. In this analysis, a three-dimensional analytical mathematical model is used to assess several aspects of americium-241 contamination of groundwater, including radioactive transformation, advection, dispersion, and soil sorption. Simulation results indicate that no significant radiological impacts would occur to the nearby residents via the groundwater pathway. 15 refs., 2 figs., 2 tabs.

  5. Oxidation of trivalent americium, curium, and terbium in solutions of sodium paratungstate

    SciTech Connect

    Fedoseev, A.M.; Krot, N.N.; Spitsyn, V.I.

    1986-09-01

    In the further study of the behavior of the actinides and lanthanides in solutions of heteropoly-compounds, the authors succeed in finding conditions under which the formation of americium (IV), curium (IV), and terbium (IV) decatungstates is observed. The results of experiments along this line are brieflyoutlined. It is shown that trivalent americium, curium, and terbium are oxidzed by heating with persulfate not only in solutions ofunsaturated heteropolytungstates but also in solutions of isopoly-compounds of tungsten. However, the degree of oxidation of curium and terbium (III) in the latter case is appreciably lover. In addition to persulfate ions, ozone can be used for the oxidation of americium (III) in solutions of sodium paratungstate.

  6. Separation and determination of americium in low-level alkaline waste of NPP origin

    NASA Astrophysics Data System (ADS)

    Todorov, B.; Djingova, R.; Nikiforova, A.

    2006-01-01

    The aim of this work is to develop a short and cost-saving procedure for the determination of 241Am in sludge sample of the alkaline low-level radioactive waste (LL LRAW) collected from Nuclear Power Plant “Kozloduy”. The determination of americium was a part of a complex analytical approach, where group actinide separation was achieved. An anion exchange was used for separation of americium from uranium, plutonium and iron. For the separation of americium extraction with diethylhexyl phosphoric acid (DEHPA) was studied. The final radioactive samples were prepared by micro co-precipitation with NdF3, counted by alpha and gamma spectrometry. The procedure takes 2 hours. The recovery yield of the procedure amounts to (95 ± 1.5)% and the detection limit is 53 mBq/kg 241Am (t=150 000 s). The analytical procedure was applied for actual liquid wastes and results were compared to standard procedure.

  7. Americium purification by a combined anion exchange and bidentate organophosphorus solvent extraction process. [Patent application

    SciTech Connect

    Navratil, J.D.; Martella, L.L.

    1981-04-10

    Americium is separated from mixtures containing plutonium, other actinides, and other non-lanthamide impurities, by a combined process of anion exchange resin sorption to remove plutonium, and a bidentate organophosphorus solvent extraction of americium of the anion exchange resin effluent. Dihexyl-N,N-diethylcarbamylmethylenephosphonate is a preferred solvent. The initial mixture may be subjected to a cation exchange operation to remove monovalent impurities. The process is especially effective when aluminum, zinc, lead, and copper are present in significant quantities in the original mixture.

  8. Synthesis of functionalised BTPhen derivatives - effects on solubility and americium extraction.

    PubMed

    Higginson, Matthew A; Kyle, Nichola D; Marsden, Olivia J; Thompson, Paul; Livens, Francis R; Heath, Sarah L

    2015-10-01

    Separation of the minor actinides (Am/Cm) from spent nuclear fuel post-PUREX process is expected to play a key part in new reprocessing methodologies. To date, a number of selective americium extractants from the BTPhen ligand family have been identified. In this investigation, we synthesise 24 novel BTPhens with additional functionality to determine the effects on solubilities and americium extraction capabilities. The data obtained will allow for tuning of steric/electronic properties of BTPhens in order to assist future extractant design. PMID:26331995

  9. Americium biokinetics in benthic organisms as a function of feeding mode

    SciTech Connect

    Fowler, S.W.; Carvalho, F.P.

    1985-12-01

    Transuranic radionuclides in the environment have arisen from nuclear weapons testing, release from nuclear waste reprocessing plants and accidents with nuclear devices. Although at present the plutonium inventory is greater than that of any other transuranium element, the americium inventory will continue to increase due to the in situ decay of SU Pu. Furthermore some studies have demonstrated that americium is more bioavailable than plutonium in aquatic environments. The authors therefore undertook to delineate, experimentally, the biokinetics of SU Am in some marine benthic species with very different feeding-digestion strategies, which hitherto have not been studied in any detail in a radioecological context.

  10. National low-level waste management program radionuclide report series, Volume 14: Americium-241

    SciTech Connect

    Winberg, M.R.; Garcia, R.S.

    1995-09-01

    This report, Volume 14 of the National Low-Level Waste Management Program Radionuclide Report Series, discusses the radiological and chemical characteristics of americium-241 ({sup 241}Am). This report also includes discussions about waste types and forms in which {sup 241}Am can be found and {sup 241}Am behavior in the environment and in the human body.

  11. Separation of Americium in High Oxidation States from Curium Utilizing Sodium Bismuthate.

    PubMed

    Richards, Jason M; Sudowe, Ralf

    2016-05-01

    A simple separation of americium from curium would support closure of the nuclear fuel cycle, assist in nuclear forensic analysis, and allow for more accurate measurement of neutron capture properties of (241)Am. Methods for the separation of americium from curium are however complicated and time-consuming due to the similar chemical properties of these elements. In this work a novel method for the separation of americium from curium in nitric acid media was developed using sodium bismuthate to perform both the oxidation and separation. Sodium bismuthate is shown to be a promising material for performing a simple and rapid separation. Curium is more strongly retained than americium on the undissolved sodium bismuthate at nitric acid concentrations below 1.0 M. A separation factor of ∼90 was obtained in 0.1 M nitric acid. This separation factor is achieved within the first minute of contact and is maintained for at least 2 h of contact. Separations using sodium bismuthate were performed using solid-liquid extraction as well as column chromatography. PMID:27079565

  12. Understanding the Chemistry of Uncommon Americium Oxidation States for Application to Actinide/Lanthanide Separations

    SciTech Connect

    Leigh Martin; Bruce J. Mincher; Nicholas C. Schmitt

    2007-09-01

    A spectroscopic study of the stability of Am(V) and Am(VI) produced by oxidizing Am(III) with sodium bismuthate is presented, varying the initial americium concentration, temperature and length of the oxidation was seen to have profound effects on the resultant solutions.

  13. Apparatus for fabrication of americium- beryllium neutron sources prevents capsule contamination

    NASA Technical Reports Server (NTRS)

    Mohr, W. C.; Van Loom, J. A.

    1967-01-01

    Modified gloved enclosure is used to fill a capsule with a mixture of americium and beryllium radioactive powders to seal weld the opening, and to test it for leaks. It contains a horizontal partition, vortex mixer, mounting press, welder, test vessel, and radiation shielding to prevent surface contamination.

  14. Environmental impacts of the release of a transuranic actinide, americium-241, from a contaminated facility

    SciTech Connect

    Want, J.; Merry-Libby, P.

    1985-10-29

    Americium-241 is widely used as a radiation source, but it also has some potential risk if taken into the body because of its high dose conversion factor. Although the radiotoxicity of americium-241 is small compared to other transuranic actinides, its effects on the reproductive system and on development of the placenta are more damaging than the effects of plutonium-239. In Ohio, a gemologist's laboratory was contaminated with americium-241. Prior to decontamination of the laboratory, potential radiological impacts to the surrounding environment were assessed. A hypothetical fire accident resulting in a unit release (1 curie) was assumed. Potential radiological impacts were simulated using an atmospheric dispersion and dosimetry model with local meteorological data, population census data, and detailed information regarding the neighborhood. The results indicate that there could have been a significant impact on nearby residents from americium-241 via atmospheric dispersion if a major catastrophic release had occurred prior to contamination and decommissioning of the laboratory. 14 refs., 3 figs., 2 tabs.

  15. The 5f localization/delocalization in square and hexagonal americium monolayers: a FP-LAPW electronic structure study

    NASA Astrophysics Data System (ADS)

    Gao, D.; Ray, A. K.

    2006-04-01

    The electronic and geometrical properties of bulk americium and square and hexagonal americium monolayers have been studied with the full-potential linearized augmented plane wave (FP-LAPW) method. The effects of several common approximations are examined: (1) non-spin polarization (NSP) vs. spin polarization (SP); (2) scalar-relativity (no spin-orbit coupling (NSO)) vs. full-relativity (i.e., with spin-orbit (SO) coupling included); (3) local-density approximation (LDA) vs. generalized-gradient approximation (GGA). Our results indicate that both spin polarization and spin orbit coupling play important roles in determining the geometrical and electronic properties of americium bulk and monolayers. A compression of both americium square and hexagonal monolayers compared to the americium bulk is also observed. In general, the LDA is found to underestimate the equilibrium lattice constant and give a larger total energy compared to the GGA calculations. While spin orbit coupling shows a similar effect on both square and hexagonal monolayer calculations regardless of the model, GGA versus LDA, an unusual spin polarization effect on both square and hexagonal monolayers is found in the LDA results as compared with the GGA results. The 5f delocalization transition of americium is employed to explain our observed unusual spin polarization effect. In addition, our results at the LDA level of theory indicate a possible 5f delocalization could happen in the americium surface within the same Am II (fcc crystal structure) phase, unlike the usually reported americium 5f delocalization which is associated with crystal structure change. The similarities and dissimilarities between the properties of an Am monolayer and a Pu monolayer are discussed in detail.

  16. 10 CFR 31.8 - Americium-241 and radium-226 in the form of calibration or reference sources.

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... 10 Energy 1 2010-01-01 2010-01-01 false Americium-241 and radium-226 in the form of calibration or reference sources. 31.8 Section 31.8 Energy NUCLEAR REGULATORY COMMISSION GENERAL DOMESTIC LICENSES FOR BYPRODUCT MATERIAL § 31.8 Americium-241 and radium-226 in the form of calibration or reference sources. (a) A general license is issued to...

  17. Solid-liquid separation of oxidized americium from fission product lanthanides

    NASA Astrophysics Data System (ADS)

    Shehee, T. C.; Martin, L. R.; Nash, K. L.

    2010-03-01

    The separation of americium from the lanthanides and curium is a requirement if transmutation of americium is to be performed in advanced nuclear fuel cycles. Oxidation of Am3+ to AmO2+ or AmO22+ may allow separation of Am from Ln and Cm in one step, since the lanthanides and curium do not have higher oxidation states as accessible. Two possible solid-liquid separation methods have been developed to address this difficult separation. Under acidic conditions using oxone or persulfate, the oxidation and retention of tracer Am in the aqueous phase has been observed with a separation factor of 11 ± 1. Most of these studies have been conducted using 237NpO2(NO3), 233UO2(NO3)2, 238Pu(NO3)4 and 241Am(NO3)3 at radiotracer concentrations. Lanthanides precipitate as the sodium or potassium europium double sulfate salt. Under basic conditions, ozone oxidation of Am(CO3)OH(s) solubilizes Am from a lanthanide carbonate hydroxide solid phase to the aqueous phase as the AmO2(CO3)34-or AmO2(CO3)35- species. For the ozone oxidation of the americium tracer a separation factor of 1.6 ± 0.8 and 47 ± 2 for the oxidation/separation in Na2CO3 and NaHCO3 respectively.

  18. Structure of a single model to describe plutonium and americium decorporation by DTPA treatments.

    PubMed

    Fritsch, P; Sérandour, A L; Grémy, O; Phan, G; Tsapis, N; Fattal, E; Benech, H; Deverre, J R; Poncy, J L

    2010-10-01

    The aim of this study is to propose a single modeling structure to describe both plutonium and americium decorporation by DTPA, which is based on hypotheses mostly validated by experimental data. Decorporation efficacy of extracellular retention depends on the concentration ratio of DTPA vs. actinides and varies in each compartment according to the amount of biological ligands and their affinity for actinides. By contrast, because the relatively long residence time of DTPA after its cell internalization and the stability of actinide-DTPA complexes, intracellular decorporation efficacy is mainly controlled by a DTPA/actinide ratio, which is specific to each retention compartment. Although the affinity of DTPA is much lower for americium than for plutonium, a larger decorporation of americium can be obtained, which is explained by different biological ligands and/or their affinity for the actinide. Altogether, these results show that the relative contribution of intra vs. extracellular decorporation varies depending on the actinide, the chemical form of radionuclides, the galenic formulation of DTPA, and the treatment schedule. PMID:20838098

  19. Influence of dissolved organic substances in groundwater on sorption behavior of americium and neptunium

    SciTech Connect

    Boggs, S. Jr.; Seitz, M.G.

    1984-01-01

    Groundwaters typically contain dissolved organic carbon consisting largely of high molecular weight compounds of humic and fulvic acids. To evaluate whether these dissolved organic substances can enhance the tranport of radionuclides through the groundwater system, experiments were conducted to examine the sorption of americium and neptunium onto crushed basalt in the presence of dissolved humic- and fulvic-acid organic carbon introduced into synthetic groundwater. The partitioning experiments with synthetic groundwater show that increasing the concentration of either humic or fulvic acid in the water has a significant inhibiting effect on sorption of both americium and neptunium. At 22/sup 0/C, adsorption of these radionuclides, as measured by distribution ratios (the ratio of nuclide sorbed onto the solid to nuclide in solution at the end of the experiment), decreased by 25% to 50% by addition of as little as 1 mg/L dissolved organic carbon and by one to two orders of magnitude by addition of 100 to 200 mg/L dissolved organic carbon. Distribution ratios measured in solutions reacted at 90/sup 0/C similarly decreased with the addition of dissolved organic carbon but generally ranged from one to two orders of magnitude higher than those determined in the 22/sup 0/C experiment. These results suggest that organic carbon dissolved in deep groundwaters may significantly enhance the mobility of radionuclides of americium and neptunium. 23 references, 5 figures, 11 tables.

  20. Fabrication of uranium-americium mixed oxide pellet from microsphere precursors: Application of CRMP process

    NASA Astrophysics Data System (ADS)

    Remy, E.; Picart, S.; Delahaye, T.; Jobelin, I.; Lebreton, F.; Horlait, D.; Bisel, I.; Blanchart, P.; Ayral, A.

    2014-10-01

    Mixed uranium-americium oxides are one of the materials envisaged for Americium Bearing Blankets dedicated to transmutation in fast neutron reactors. Recently, several processes have been developed in order to validate fabrication flowchart in terms of material specifications such as density and homogeneity but also to suggest simplifications for lowering industrial costs and hazards linked to dust generation of highly contaminating and irradiating compounds. This study deals with the application of an innovative route using mixed oxide microspheres obtained from metal loaded resin bead calcination, called Calcined Resin Microsphere Pelletization (CRMP). The synthesis of mixed oxide microsphere precursor of U0.9Am0.1O2±δ is described as well as its characterisation. The use of this free-flowing precursor allows the pressing and sintering of one pellet of U0.9Am0.1O2±δ. The ceramic obtained was characterised and results showed that its microstructure is dense and homogeneous and its density attains 95% of the theoretical density. This study validates the scientific feasibility of the CRMP process applied to the fabrication of uranium and americium-containing materials.

  1. Americium characterization by X-ray fluorescence and absorption spectroscopy in plutonium uranium mixed oxide

    SciTech Connect

    Degueldre, Claude Cozzo, Cedric; Martin, Matthias; Grolimund, Daniel; Mieszczynski, Cyprian

    2013-06-01

    Plutonium uranium mixed oxide (MOX) fuels are currently used in nuclear reactors. The actinides in these fuels need to be analyzed after irradiation for assessing their behaviour with regard to their environment and the coolant. In this work the study of the atomic structure and next-neighbour environment of Am in the (Pu,U)O₂ lattice in an irradiated (60 MW d kg⁻¹) MOX sample was performed employing micro-X-ray fluorescence (µ-XRF) and micro-X-ray absorption fine structure (µ-XAFS) spectroscopy. The chemical bonds, valences and stoichiometry of Am (~0.66 wt%) are determined from the experimental data gained for the irradiated fuel material examined in its peripheral zone (rim) of the fuel. In the irradiated sample Am builds up as Am³⁺ species within an [AmO₈]¹³⁻ coordination environment (e.g. >90%) and no (<10%) Am(IV) or (V) can be detected in the rim zone. The occurrence of americium dioxide is avoided by the redox buffering activity of the uranium dioxide matrix. - Graphical abstract: Americium LIII XAFS spectra recorded for the irradiated MOX sub-sample in the rim zone for a 300 μm×300 μm beam size area investigated over six scans of 4 h. The records remain constant during multi-scan. The analysis of the XAFS signal shows that Am is found as trivalent in the UO₂ matrix. This analytical work shall open the door of very challenging analysis (speciation of fission product and actinides) in irradiated nuclear fuels. - Highlights: • Americium was characterized by microX-ray absorption spectroscopy in irradiated MOX fuel. • The americium redox state as determined from XAS data of irradiated fuel material was Am(III). • In the sample, the Am³⁺ face an AmO₈¹³⁻coordination environment in the (Pu,U)O₂ matrix. • The americium dioxide is reduced by the uranium dioxide matrix.

  2. Isotopic Biogeochemistry

    NASA Technical Reports Server (NTRS)

    Hayes, J. M.

    1985-01-01

    An overview is provided of the biogeochemical research. The funding, productivity, personnel and facilities are reviewed. Some of the technical areas covered are: carbon isotopic records; isotopic studies of banded iron formations; isotope effects in microbial systems; studies of organic compounds in ancient sediments; and development in isotopic geochemistry and analysis.

  3. Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

    PubMed

    León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D

    2009-04-01

    New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with

  4. Speciation of americium in seawater and accumulation in the marine sponge Aplysina cavernicola.

    PubMed

    Maloubier, Melody; Michel, Hervé; Solari, Pier Lorenzo; Moisy, Philippe; Tribalat, Marie-Aude; Oberhaensli, François R; Dechraoui Bottein, Marie Yasmine; Thomas, Olivier P; Monfort, Marguerite; Moulin, Christophe; Den Auwer, Christophe

    2015-12-21

    The fate of radionuclides in the environment is a cause of great concern for modern society, seen especially in 2011 after the Fukushima accident. Among the environmental compartments, seawater covers most of the earth's surface and may be directly or indirectly impacted. The interaction between radionuclides and the marine compartment is therefore essential for better understanding the transfer mechanisms from the hydrosphere to the biosphere. This information allows for the evaluation of the impact on humans via our interaction with the biotope that has been largely undocumented up to now. In this report, we attempt to make a link between the speciation of heavy elements in natural seawater and their uptake by a model marine organism. More specifically, because the interaction of actinides with marine invertebrates has been poorly studied, the accumulation in a representative member of the Mediterranean coralligenous habitat, the sponge Aplysina cavernicola, was investigated and its uptake curve exposed to a radiotracer (241)Am was estimated using a high-purity Ge gamma spectrometer. But in order to go beyond the phenomenological accumulation rate, the speciation of americium(III) in seawater must be assessed. The speciation of (241)Am (and natural europium as its chemically stable surrogate) in seawater was determined using a combination of different techniques: Time-Resolved Laser-Induced Fluorescence (TRLIF), Extended X-ray Absorption Fine Structure (EXAFS) at the LIII edge, Attenuated Total Reflectance Fourier Transform Infrared (ATR-FTIR) spectroscopy and Scanning Electron Microscopy (SEM) and the resulting data were compared with the speciation modeling. In seawater, the americium(III) complex (as well as the corresponding europium complex, although with conformational differences) was identified as a ternary sodium biscarbonato complex, whose formula can be tentatively written as NaAm(CO3)2·nH2O. It is therefore this chemical form of americium that is

  5. Production of films of uranium and americium compounds by thermal decomposition of volatile β-diketonates

    NASA Astrophysics Data System (ADS)

    Danilin, I. D.; Kartushin, V. D.; Pilipenko, N. V.; Abramycheva, I. D.; Vesnovskii, S. P.

    2002-03-01

    The production of films containing uranium and americium through thermal decomposition of diketonates and their adducts is described. It is demonstrated that for substrate temperatures in the range 300-400°C and at a residual reactor pressure of 1.3 Pa, stable uranium-containing layers up to several milligrams per square centimetre can be produced, with yields of up to 90%. A variety of metal backings were investigated, including aluminium and its alloys, stainless steel and titanium. Similar results were obtained for americium, but with a strong influence of backing material on the yield. X-ray diffraction identified the chemical form of the uranium deposits as dioxide, with crystal lattice parameters varying from 5.4338 to 5.4871 Å, while the density determined by X-rays lies within the range from 10920 to 11255 kg/m 3. In the case of Am (Cm) hexafluoroacetyl acetonate decomposition, the deposit is most probably AmF 3 (CmF 3). The gases released from the pyrolytic uranium dioxide layers heated in vacuum to 470°C were studied. The volume of gas released varied between 10 and 40 cm 3 per gram of UO 2 depending on the initial β-diketonate preparation and reagent purity. The released gases were mainly hydrogen, carbon monoxide, carbon dioxide, water and a small amount of methane. The films of uranium and americium obtained by thermal decomposition show good adhesion to backings and are suitable for use in a number of fields, for example in nuclear physics research and instrument engineering.

  6. Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids.

    PubMed

    Dittrich, Timothy Mark; Boukhalfa, Hakim; Ware, Stuart Douglas; Reimus, Paul William

    2015-10-01

    Understanding the parameters that control colloid-mediated transport of radionuclides is important for the safe disposal of used nuclear fuel. We report an experimental and reactive transport modeling examination of americium transport in a groundwater-bentonite-fracture fill material system. A series of batch sorption and column transport experiments were conducted to determine the role of desorption kinetics from bentonite colloids in the transport of americium through fracture materials. We used fracture fill material from a shear zone in altered granodiorite collected from the Grimsel Test Site (GTS) in Switzerland and colloidal suspensions generated from FEBEX bentonite, a potential repository backfill material. The colloidal suspension (100 mg L(-1)) was prepared in synthetic groundwater that matched the natural water chemistry at GTS and was spiked with 5.5 × 10(-10) M (241)Am. Batch characterizations indicated that 97% of the americium in the stock suspension was adsorbed to the colloids. Breakthrough experiments conducted by injecting the americium colloidal suspension through three identical columns in series, each with mean residence times of 6 h, show that more than 95% of the bentonite colloids were transported through each of the columns, with modeled colloid filtration rates (k(f)) of 0.01-0.02 h(-1). Am recoveries in each column were 55-60%, and Am desorption rate constants from the colloids, determined from 1-D transport modeling, were 0.96, 0.98, and 0.91 h(-1) in the three columns, respectively. The consistency in Am recoveries and desorption rate constants in each column indicates that the Am was not associated with binding sites of widely-varying strengths on the colloids, as one binding site with fast kinetics represented the system accurately for all three sequential columns. Our data suggest that colloid-mediated transport of Am in a bentonite-fracture fill material system is unlikely to result in transport over long distance scales because

  7. Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids

    DOE PAGESBeta

    Dittrich, Timothy Mark; Boukhalfa, Hakim; Ware, Stuart Douglas; Reimus, Paul William

    2015-07-13

    Understanding the parameters that control colloid-mediated transport of radionuclides is important for the safe disposal of used nuclear fuel. We report an experimental and reactive transport modeling examination of americium transport in a groundwater–bentonite–fracture fill material system. A series of batch sorption and column transport experiments were conducted to determine the role of desorption kinetics from bentonite colloids in the transport of americium through fracture materials. We used fracture fill material from a shear zone in altered granodiorite collected from the Grimsel Test Site (GTS) in Switzerland and colloidal suspensions generated from FEBEX bentonite, a potential repository backfill material. Themore » colloidal suspension (100 mg L–1) was prepared in synthetic groundwater that matched the natural water chemistry at GTS and was spiked with 5.5 × 10–10 M241Am. Batch characterizations indicated that 97% of the americium in the stock suspension was adsorbed to the colloids. Breakthrough experiments conducted by injecting the americium colloidal suspension through three identical columns in series, each with mean residence times of 6 h, show that more than 95% of the bentonite colloids were transported through each of the columns, with modeled colloid filtration rates (kf) of 0.01–0.02 h–1. Am recoveries in each column were 55–60%, and Am desorption rate constants from the colloids, determined from 1-D transport modeling, were 0.96, 0.98, and 0.91 h–1 in the three columns, respectively. The consistency in Am recoveries and desorption rate constants in each column indicates that the Am was not associated with binding sites of widely-varying strengths on the colloids, as one binding site with fast kinetics represented the system accurately for all three sequential columns. As a result, our data suggest that colloid-mediated transport of Am in a bentonite-fracture fill material system is unlikely to result in transport over long

  8. Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids

    SciTech Connect

    Dittrich, Timothy Mark; Boukhalfa, Hakim; Ware, Stuart Douglas; Reimus, Paul William

    2015-07-13

    Understanding the parameters that control colloid-mediated transport of radionuclides is important for the safe disposal of used nuclear fuel. We report an experimental and reactive transport modeling examination of americium transport in a groundwater–bentonite–fracture fill material system. A series of batch sorption and column transport experiments were conducted to determine the role of desorption kinetics from bentonite colloids in the transport of americium through fracture materials. We used fracture fill material from a shear zone in altered granodiorite collected from the Grimsel Test Site (GTS) in Switzerland and colloidal suspensions generated from FEBEX bentonite, a potential repository backfill material. The colloidal suspension (100 mg L–1) was prepared in synthetic groundwater that matched the natural water chemistry at GTS and was spiked with 5.5 × 10–10 M241Am. Batch characterizations indicated that 97% of the americium in the stock suspension was adsorbed to the colloids. Breakthrough experiments conducted by injecting the americium colloidal suspension through three identical columns in series, each with mean residence times of 6 h, show that more than 95% of the bentonite colloids were transported through each of the columns, with modeled colloid filtration rates (kf) of 0.01–0.02 h–1. Am recoveries in each column were 55–60%, and Am desorption rate constants from the colloids, determined from 1-D transport modeling, were 0.96, 0.98, and 0.91 h–1 in the three columns, respectively. The consistency in Am recoveries and desorption rate constants in each column indicates that the Am was not associated with binding sites of widely-varying strengths on the colloids, as one binding site with fast kinetics represented the system accurately for all three sequential columns. As a result, our data suggest that colloid-mediated transport of Am in a bentonite-fracture fill

  9. Comparison of acid leachate and fusion methods to determine plutonium and americium in environmental samples

    SciTech Connect

    Smith, L.L.; Markun, F.; TenKate, T.

    1992-06-01

    The Analytical Chemistry Laboratory at Argonne National Laboratory performs radiochemical analyses for a wide variety of sites within the Department of Energy complex. Since the chemical history of the samples may vary drastically from site to site, the effectiveness of any analytical technique may also vary. This study compares a potassium fluoride-pyrosulfate fusion technique with an acid leachate method. Both normal and high-fired soils and vegetation samples were analyzed for both americium and plutonium. Results show both methods work well, except for plutonium in high-fired soils. Here the fusion method provides higher accuracy.

  10. Magnetic Polarization of the Americium J =0 Ground State in AmFe2

    NASA Astrophysics Data System (ADS)

    Magnani, N.; Caciuffo, R.; Wilhelm, F.; Colineau, E.; Eloirdi, R.; Griveau, J.-C.; Rusz, J.; Oppeneer, P. M.; Rogalev, A.; Lander, G. H.

    2015-03-01

    Trivalent americium has a nonmagnetic (J =0 ) ground state arising from the cancellation of the orbital and spin moments. However, magnetism can be induced by a large molecular field if Am3 + is embedded in a ferromagnetic matrix. Using the technique of x-ray magnetic circular dichroism, we show that this is the case in AmFe2 . Since ⟨Jz⟩=0 , the spin component is exactly twice as large as the orbital one, the total Am moment is opposite to that of Fe, and the magnetic dipole operator ⟨Tz⟩ can be determined directly; we discuss the progression of the latter across the actinide series.

  11. Americium/europium separation by synergistic extraction mixtures of bis-tetrazolyl pyridines with chlorinated cobalt dicarbollide

    SciTech Connect

    Smirnov, I.V.; Babain, V.A.; Chirkov, A.V.

    2008-07-01

    Americium and europium extraction by synergistic mixtures of 2,6-bis(1-aryl-1 H-tetrazol-5-yl)pyridines (ATP) with chlorinated cobalt dicarbollide (CCD) in polar diluents from acidic media was studied. The effect of diluent, composition of aqueous phase, and substituent nature in the aryl ring of ATPs on the extraction efficiency and selectivity of americium and europium separation was investigated. The Am-Eu separation factor was close to 100 at the optimal ratio of ATPs:CCD {approx}1:1 in the synergistic mixture. High resistance of 2,6-bis-aryl-tetrazolyl pyridines to the action of acids and radiolysis was demonstrated. (authors)

  12. Comparative skeletal distribution of americium and plutonium in man, monkey and baboon

    SciTech Connect

    Lynch, T.P.; Dagle, G.E.; Kathren, R.L.; McInroy, J.F.

    1988-10-01

    The skeletal distributions of americium and plutonium in four humans were compared with the skeletal distributions of these radioelements in baboons and monkeys. With respect to the skeletal distribution of these elements, excellent agreement was noted among the four human cases; americium data was available for all four cases and plutonium for three. The human case database was thus adequate for comparison with those of other primates. A statistically significant correlation was found between the /sup 241/Am and /sup 239/Pu + /sup 240/Pu skeletal distributions in the humans and those in non-human primates. Trabecular bone had the highest concentrations of /sup 241/Am and /sup 239 +240/Pu in man, baboon, and monkey. Scaling factors are proposed to convert the percentages of skeletal activity in animal bones to the corresponding percentages in the bones of the human skeleton. However, considerable variation was found between the humans and animals in the percentages of the skeletal activity found in the same bone. 12 refs., 7 tabs.

  13. Evaluation of americium-241 toxicity influence on the microbial growth of organic wastes

    SciTech Connect

    Takehiro Marumo, Julio; Padua Ferreira, Rafael Vicente de; Keiko Isiki, Vera Lucia; Miyamoto, Hissae; Sayuri Takara, Aline; Kazumi Sakata, Solange; Bellini, Maria Helena; Cardoso Pedroso de Lima, Luis Filipe

    2007-07-01

    Available in abstract form only. Full text of publication follows: Since the licenses for using radioactive sources in radioactive lightning rods were lifted by the Brazilian national nuclear authority, in 1989, the radioactive devices have been replaced by Franklin type and collected as radioactive waste. However, only 20 percent of the estimated total number of installed rods was delivered to Brazilian Nuclear Commission. This situation causes concern, due to, first, the possibility of the rods being disposed as domestic waste, and second, the americium, the most commonly employed radionuclide, is classified as a high-toxicity element. In the present study, Am-241 migration experiments were performed by a lysimeter system, in order to evaluate the risk of contamination caused by radioactive lightning rods disposed as a common solid waste. Besides the risk evaluation, it is important to know the mechanism of the Am-241 release or retention in waste as well as its influence in the waste decomposition processes. Many factors are involved, but microorganisms present in the waste play an important role in its degradation, which control the physical and chemical processes. The objective of this work was to evaluate the Am-241 influence on the microbial population by counting number of cells in lysimeters leachate. Preliminary results suggest that americium may influence significantly the bacteria growth in organic waste, evidenced by culture under aerobiosis and an-aerobiosis and the antimicrobial resistance test. (authors)

  14. An economic analysis of a light and heavy water moderated reactor synergy: burning americium using recycled uranium

    SciTech Connect

    Wojtaszek, D.; Edwards, G.

    2013-07-01

    An economic analysis is presented for a proposed synergistic system between 2 nuclear utilities, one operating light water reactors (LWR) and another running a fleet of heavy water moderated reactors (HWR). Americium is partitioned from LWR spent nuclear fuel (SNF) to be transmuted in HWRs, with a consequent averted disposal cost to the LWR operator. In return, reprocessed uranium (RU) is supplied to the HWRs in sufficient quantities to support their operation both as power generators and americium burners. Two simplifying assumptions have been made. First, the economic value of RU is a linear function of the cost of fresh natural uranium (NU), and secondly, plutonium recycling for a third utility running a mixed oxide (MOX) fuelled reactor fleet has been already taking place, so that the extra cost of americium recycling is manageable. We conclude that, in order for this scenario to be economically attractive to the LWR operator, the averted disposal cost due to partitioning americium from LWR spent fuel must exceed 214 dollars per kg, comparable to estimates of the permanent disposal cost of the high level waste (HLW) from reprocessing spent LWR fuel. (authors)

  15. Ditopic CMPO-pillar[5]arenes as unique receptors for efficient separation of americium(III) and europium(III).

    PubMed

    Fang, Yuyu; Yuan, Xiangyang; Wu, Lei; Peng, Zhiyong; Feng, Wen; Liu, Ning; Xu, Dingguo; Li, Shoujian; Sengupta, Arijit; Mohapatra, Prasanta K; Yuan, Lihua

    2015-03-11

    A unique host-guest recognition process involving a new class of homoditopic CMPO-pillar[5]arenes and lanthanides was revealed to proceed in a stepwise manner, and correlated with the efficient separation of americium(III) and europium(III) under acidic feed conditions. PMID:25671799

  16. XRD monitoring of α self-irradiation in uranium-americium mixed oxides.

    PubMed

    Horlait, Denis; Lebreton, Florent; Roussel, Pascal; Delahaye, Thibaud

    2013-12-16

    The structural evolution under (241)Am self-irradiation of U(1-x)Am(x)O(2±δ) transmutation fuels (with x ≤ 0.5) was studied by X-ray diffraction (XRD). Samples first underwent a preliminary heat treatment performed under a reducing atmosphere (Ar/H2(4%)) aiming to recover the previously accumulated structural defects. Over all measurements (carried out over up to a full year and for integrated doses up to 1.5 × 10(18) α-decay events·g(-1)), only fluorite U(1-x)Am(x)O(2±δ) solid solutions were observed. Within a few days after the end of the heat treatment, each of the five studied samples was slowly oxidized as a consequence of their move to air atmosphere, which is evidenced by XRD by an initial sharp decrease of the unit cell parameter. For the compounds with x ≤ 0.15, this oxidation occurred without any phase transitions, but for U0.6Am0.4O(2±δ) and U0.5Am0.5O(2±δ), this process is accompanied by a transition from a first fluorite solid solution to a second oxidized one, as the latter is thermodynamically stable in ambient conditions. In the meantime and after the oxidation process, (241)Am α self-irradiation caused a structural swelling up to ∼0.8 vol %, independently of the sample composition. The kinetic constants of swelling were also determined by regression of experimental data and are, as expected, dependent on x and thus on the dose rate. The normalization of these kinetic constants by sample α-activity, however, leads to very close swelling rates among the samples. Finally, evolutions of microstrain and crystallite size were also monitored, but for the considered dose rates and cumulated doses, α self-irradiation was found, within the limits of the diffractometer used, to have almost no impact on these characteristics. Microstrain was found to be influenced instead by the americium content in the materials (i.e., by the impurities associated with americium starting material and the increase of cationic charge heterogeneity with

  17. Isotope separation

    DOEpatents

    Bartlett, Rodney J.; Morrey, John R.

    1978-01-01

    A method and apparatus is described for separating gas molecules containing one isotope of an element from gas molecules containing other isotopes of the same element in which all of the molecules of the gas are at the same electronic state in their ground state. Gas molecules in a gas stream containing one of the isotopes are selectively excited to a different electronic state while leaving the other gas molecules in their original ground state. Gas molecules containing one of the isotopes are then deflected from the other gas molecules in the stream and thus physically separated.

  18. Transportability Class of Americium in K Basin Sludge under Ambient and Hydrothermal Processing Conditions

    SciTech Connect

    Delegard, Calvin H.; Schmitt, Bruce E.; Schmidt, Andrew J.

    2006-08-01

    This report establishes the technical bases for using a ''slow uptake'' instead of a ''moderate uptake'' transportability class for americium-241 (241Am) for the K Basin Sludge Treatment Project (STP) dose consequence analysis. Slow uptake classes are used for most uranium and plutonium oxides. A moderate uptake class has been used in prior STP analyses for 241Am based on the properties of separated 241Am and its associated oxide. However, when 241Am exists as an ingrown progeny (and as a small mass fraction) within plutonium mixtures, it is appropriate to assign transportability factors of the predominant plutonium mixtures (typically slow) to the Am241. It is argued that the transportability factor for 241Am in sludge likewise should be slow because it exists as a small mass fraction as the ingrown progeny within the uranium oxide in sludge. In this report, the transportability class assignment for 241Am is underpinned with radiochemical characterization data on K Basin sludge and with studies conducted with other irradiated fuel exposed to elevated temperatures and conditions similar to the STP. Key findings and conclusions from evaluation of the characterization data and published literature are summarized here. Plutonium and 241Am make up very small fractions of the uranium within the K Basin sludge matrix. Plutonium is present at about 1 atom per 500 atoms of uranium and 241Am at about 1 atom per 19000 of uranium. Plutonium and americium are found to remain with uranium in the solid phase in all of the {approx}60 samples taken and analyzed from various sources of K Basin sludge. The uranium-specific concentrations of plutonium and americium also remain approximately constant over a uranium concentration range (in the dry sludge solids) from 0.2 to 94 wt%, a factor of {approx}460. This invariability demonstrates that 241Am does not partition from the uranium or plutonium fraction for any characterized sludge matrix. Most of the K Basin sludge characterization

  19. The Role of Colloids in the Transport of Plutonium and Americium: Implications for

    SciTech Connect

    Kersting, A B

    2003-09-17

    Colloids are small particulates (ranging in size from 1 to 0.001 micron) composed of inorganic and organic material and found in all natural water. Due to their small size, they have the ability to remain suspended in water and transported. Small amounts of plutonium (Pu) and americium (Am) can adsorb (attach) to colloids, and/or form colloidal-sized polymers and migrate in water. At Rocky Flats Environmental Technology Site (RFETS) sedimentation and resuspension of particulates and colloids in surface waters represent the dominant process for Pu and Am migration. The amount of Pu and Am that can be transported at RFETS has been quantified in the Pathway Analysis Report. The Pathway Analysis Report shows that the two dominant pathways for Pu and Am transport at RFETS are air and surface water. Shallow groundwater and biological pathways are minor.

  20. Imitators of plutonium and americium in a mixed uranium- plutonium nitride fuel

    NASA Astrophysics Data System (ADS)

    Nikitin, S. N.; Shornikov, D. P.; Tarasov, B. A.; Baranov, V. G.; Burlakova, M. A.

    2016-04-01

    Uranium nitride and mix uranium nitride (U-Pu)N is most popular nuclear fuel for Russian Fast Breeder Reactor. The works in hot cells associated with the radiation exposure of personnel and methodological difficulties. To know the main physical-chemical properties of uranium-plutonium nitride it necessary research to hot cells. In this paper, based on an assessment of physicochemical and thermodynamic properties of selected simulators Pu and Am. Analogues of Pu is are Ce and Y, and analogues Am - Dy. The technique of obtaining a model nitride fuel based on lanthanides nitrides and UN. Hydrogenation-dehydrogenation- nitration method of derived powders nitrides uranium, cerium, yttrium and dysprosium, held their mixing, pressing and sintering, the samples obtained model nitride fuel with plutonium and americium imitation. According to the results of structural studies have shown that all the samples are solid solution nitrides rare earth (REE) elements in UN.

  1. Magnetic polarization of the americium J=0 ground state in AmFe(2).

    PubMed

    Magnani, N; Caciuffo, R; Wilhelm, F; Colineau, E; Eloirdi, R; Griveau, J-C; Rusz, J; Oppeneer, P M; Rogalev, A; Lander, G H

    2015-03-01

    Trivalent americium has a nonmagnetic (J=0) ground state arising from the cancellation of the orbital and spin moments. However, magnetism can be induced by a large molecular field if Am^{3+} is embedded in a ferromagnetic matrix. Using the technique of x-ray magnetic circular dichroism, we show that this is the case in AmFe_{2}. Since ⟨J_{z}⟩=0, the spin component is exactly twice as large as the orbital one, the total Am moment is opposite to that of Fe, and the magnetic dipole operator ⟨T_{z}⟩ can be determined directly; we discuss the progression of the latter across the actinide series. PMID:25793847

  2. Aqueous complexes for efficient size-based separation of americium from curium.

    PubMed

    Jensen, Mark P; Chiarizia, Renato; Shkrob, Ilya A; Ulicki, Joseph S; Spindler, Brian D; Murphy, Daniel J; Hossain, Mahmun; Roca-Sabio, Adrián; Platas-Iglesias, Carlos; de Blas, Andrés; Rodríguez-Blas, Teresa

    2014-06-16

    Complexation of the adjacent actinide ions americium(III) and curium(III) by the ligand N,N'-bis[(6-carboxy-2-pyridyl)methyl]-1,10-diaza-18-crown-6 (H2bp18c6) in aqueous solution was studied to quantify and characterize its americium/curium selectivity. Liquid-liquid extraction and spectrophotometric titration indicated the presence of both fully deprotonated and monoprotonated complexes, An(bp18c6)(+) and An(Hbp18c6)(2+) (An = Am or Cm), at the acidities that would be encountered when treating nuclear wastes. The stability constants of the complexes in 1 M NaNO3 determined using competitive complexation were log β101 = 15.49 ± 0.06 for Am and 14.88 ± 0.03 for Cm, indicating a reversal of the usual order of complex stability, where ligands bind the smaller Cm(III) ion more tightly than Am(III). The Am/Cm selectivity of bp18c6(2-) that is defined by the ratio of the Am and Cm stability constants (β101 Am/β101 Cm = 4.1) is the largest reported so far for binary An(III)-ligand complexes. Theoretical density functional theory calculations using the B3LYP functional suggest that the ligand's size-selectivity for larger 4f- and 5f-element cations arises from steric constraints in the crown ether ring. Enhanced 5f character in molecular orbitals involving actinide-nitrogen interactions is predicted to favor actinide(III) complexation by bp18c6(2-) over the complexation of similarly sized lanthanide(III) cations. PMID:24890863

  3. High Purity Americium-241 for Fuel Cycle R&D Program

    SciTech Connect

    Dr. Paul A. Lessing

    2011-07-01

    Previously the U.S. Department of Energy released Am-241 for various applications such as smoke detectors and Am-Be neutron sources for oil wells. At this date there is a shortage of usable, higher purity Am-241 in metal and oxide form available in the United States. Recently, the limited source of Am-241 has been from Russia with production being contracted to existing customers. The shortage has resulted in the price per gram rising dramatically over the last few years. DOE-NE currently has need for high purity Am-241 metal and oxide to fabricate fuel pellets for reactor testing in the Fuel Cycle R&D program. All the available high purity americium has been gathered from within the DOE system of laboratories. However, this is only a fraction of the projected needs of FCRD over the next 10 years. Therefore, FCR&D has proposed extraction and purification concepts to extract Am-241 from a mixed AmO2-PuO2 feedstock stored at the Savannah River Site. The most simple extraction system is based upon high temperature reduction using lanthanum metal with concurrent evaporation and condensation to produce high purity Am metal. Metallic americium has over a four order of magnitude higher vapor pressure than plutonium. Results from small-scale reduction experiments are presented. These results confirm thermodynamic predictions that at 1000 deg C metallic lanthanum reduces both PuO2 and AmO2. Faster kinetics are expected for temperatures up to about 1500 deg C.

  4. Thermodynamic properties for rare earths and americium in pyropartitioning process solvents

    SciTech Connect

    Fusselman, S.P.; Roy, J.J.; Grimmett, D.L.

    1999-07-01

    The design of a molten metal-molten salt based chemical and electrochemical process for separation of actinides from plutonium-uranium extraction waste requires a consistent set of thermodynamic properties for the actinides and rare earths present in nuclear waste. Standard potential data for Y, La, Ce, Pr, and Gd in molten LiCl-KCl were obtained. Americium data obtained were standard potentials in molten LiCl-KCl and activity coefficients for Cd and Bi. Data were obtained between 400 and 500 C. Results for the rare earth chlorides using an improved experimental technique were consistent with theory, with standard free energy of formation values somewhat more negative than those found in the literature. Special attention was given to Am in the LiCl-KCl/Cd system because it can exist as the +2 and/or +3 ion in this system. Americium ions existed only as the +3 ion in LiCl-KCl/Bi. Standard electrochemical potentials for Am/Am{sup +2} in LiCl-KCl eutectic at 400, 450, and 500 C were {minus}2.893, {minus}2.853, and {minus}2.838 V, respectively, relative to Cl{sup 2}/Cl{sup {minus}}. Standard electrochemical potentials vs. Cl{sub 2}/Cl{sup {minus}} for Am/Am{sup +3} in LiCl-KCl eutectic were {minus}2.83 V at 450 C and {minus}2.78 V at 500 C. Activity coefficients for Am in molten Cd were 1 {times} 10{sup {minus}5} and 8 {times} 10{sup {minus}5} at 450 and 500 C.

  5. The solvent extraction of Americium(III) by 2,6-bis[(diphenylphosphino)-methyl]pyridine N,P,P` trioxide from nitric acid and hydrochloric acid solutions

    SciTech Connect

    Bond, E.M.; Engelhardt, U.; Deere, T.P.; Rapko, B.M.; Paine, R.T.

    1997-12-31

    The liquid/liquid extractions of Am(III) from nitric acid and hydrochloric acid solutions with chloroform solutions of 2,6-bis[(diphenylphosphino)methyl]pyridine N,P,P{prime} trioxide will be described. Americium(III) extracts well from high concentration nitric acid solutions (D>3000 at 6M nitric acid) and can be back extracted from the organic phase at 0.01M Nitric Acid. Americium(III) exhibits modest extraction from hydrochloric acid solutions (D=2.2 at 5M hydrochloric acid) and can be back extracted from the organic phase at 0.1M hydrochloric acid. The ligand dependency data suggest that two ligand molecules are coordinated to americium in the nitric acid system and three ligand molecules are coordinated to the americium in the hydrochloric acid system.

  6. Extraction and recovery of plutonium and americium from nitric acid waste solutions by the TRUEX process - continuing development studies

    SciTech Connect

    Leonard, R.A.; Vandegrift, G.F.; Kalina, D.G.; Fischer, D.F.; Bane, R.W.; Burris, L.; Horwitz, E.P.; Chiarisia, R.; Diamond, H.

    1985-09-01

    This report summarizes the work done to date on the application of the TRUEX solvent extraction process for removing and separately recovering plutonium and americium from a nitric acid waste solution containing these elements, uranium, and a complement of inert metal ions. This simulated waste stream is typical of a raffinate from a tributyl phosphate (TBP)-based solvent extraction process for removing uranium and plutonium from dissolved plutonium-containing metallurgical scrap. The TRUEX process solvent in these experiments was a solution of TBP and octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) dissolved in carbon tetrachloride. A flowsheet was designed on the basis of measured batch distribution ratios to reduce the TRU content of the solidified raffinate to less than or equal to 10 nCi/g and was tested in a countercurrent experiment performed in a 14-stage Argonne-model centrifugal contractor. The process solvent was recycled without cleanup. An unexpectedly high evaporative loss of CCl/sub 4/ resulted in concentration of the active extractant, CMPO, to nearly 0.30M in the solvent. Results are consistent with this higher CMPO concentration. The raffinate contained only 2 nCi/g of TRU, but the higher CMPO concentration resulted in reduced effectiveness in the stripping of americium from the solvent. Conditions can be easily adjusted to give high yields and good separation of americium and plutonium. Experimental studies of the hydrolytic and gamma-radiolytic degradation of the TRUEX-CCl/sub 4/ showed that solvent degradation would be (1) minimal for a year of processing this typical feed, which contained no fission products, and (2) could be explained almost entirely by hydrolytic and radiolytic damage to TBP. Even for gross amounts of solvent damage, scrubbing with aqueous sodium carbonate solution restored the original americium extraction and stripping capability of the solvent. 43 refs., 5 figs., 36 tabs.

  7. Isotopic chirality

    SciTech Connect

    Floss, H.G.

    1994-12-01

    This paper deals with compounds that are chiral-at least in part, due to isotope substitution-and their use in tracing the steric course of enzyme reaction in vitro and in vivo. There are other applications of isotopically chiral compounds (for example, in analyzing the steric course of nonenzymatic reactions and in probing the conformation of biomolecules) that are important but they will not be discussed in this context.

  8. Transuranium isotopes

    SciTech Connect

    Hoffman, D.C.

    1985-12-01

    The needs of the research community for the production of transuranium isotopes, the quantities required, the continuity of production desired, and what a new steady state neutron source would have to provide to satisfy these needs are discussed. Examples of past frontier research which need these isotopes as well as an outline of the proposed Large Einsteinium Activation Program, LEAP, which requires roughly ten times the current production of /sup 254/Es are given. 15 refs., 5 figs., 4 tabs.

  9. The behaviour under irradiation of molybdenum matrix for inert matrix fuel containing americium oxide (CerMet concept)

    NASA Astrophysics Data System (ADS)

    D'Agata, E.; Knol, S.; Fedorov, A. V.; Fernandez, A.; Somers, J.; Klaassen, F.

    2015-10-01

    Americium is a strong contributor to the long term radiotoxicity of high activity nuclear waste. Transmutation by irradiation in nuclear reactors or Accelerator Driven System (ADS, subcritical reactors dedicated to transmutation) of long-lived nuclides like 241Am is therefore an option for the reduction of radiotoxicity of waste packages to be stored in a repository. In order to safely burn americium in a fast reactor or ADS, it must be incorporated in a matrix that could be metallic (CerMet target) or ceramic (CerCer target). One of the most promising matrix to incorporate Am is molybdenum. In order to address the issues (swelling, stability under irradiation, gas retention and release) of using Mo as matrix to transmute Am, two irradiation experiments have been conducted recently at the High Flux Reactor (HFR) in Petten (The Netherland) namely HELIOS and BODEX. The BODEX experiment is a separate effect test, where the molybdenum behaviour is studied without the presence of fission products using 10B to "produce" helium, the HELIOS experiment included a more representative fuel target with the presence of Am and fission product. This paper covers the results of Post Irradiation Examination (PIE) of the two irradiation experiments mentioned above where molybdenum behaviour has been deeply investigated as possible matrix to transmute americium (CerMet fuel target). The behaviour of molybdenum looks satisfying at operating temperature but at high temperature (above 1000 °C) more investigation should be performed.

  10. The behaviour under irradiation of molybdenum matrix for inert matrix fuel containing americium oxide (CerMet concept)

    NASA Astrophysics Data System (ADS)

    D'Agata, E.; Knol, S.; Fedorov, A. V.; Fernandez, A.; Somers, J.; Klaassen, F.

    2015-10-01

    Americium is a strong contributor to the long term radiotoxicity of high activity nuclear waste. Transmutation by irradiation in nuclear reactors or Accelerator Driven System (ADS, subcritical reactors dedicated to transmutation) of long-lived nuclides like 241Am is therefore an option for the reduction of radiotoxicity of waste packages to be stored in a repository. In order to safely burn americium in a fast reactor or ADS, it must be incorporated in a matrix that could be metallic (CerMet target) or ceramic (CerCer target). One of the most promising matrix to incorporate Am is molybdenum. In order to address the issues (swelling, stability under irradiation, gas retention and release) of using Mo as matrix to transmute Am, two irradiation experiments have been conducted recently at the High Flux Reactor (HFR) in Petten (The Netherland) namely HELIOS and BODEX. The BODEX experiment is a separate effect test, where the molybdenum behaviour is studied without the presence of fission products using 10B to "produce" helium, the HELIOS experiment included a more representative fuel target with the presence of Am and fission product. This paper covers the results of Post Irradiation Examination (PIE) of the two irradiation experiments mentioned above where molybdenum behaviour has been deeply investigated as possible matrix to transmute americium (CerMet fuel target). The behaviour of molybdenum looks satisfying at operating temperature but at high temperature (above 1000 °C) more investigation should be performed.

  11. Determining the americium transmutation rate and fission rate by post-irradiation examination within the scope of the ECRIX-H experiment

    NASA Astrophysics Data System (ADS)

    Lamontagne, J.; Pontillon, Y.; Esbelin, E.; Béjaoui, S.; Pasquet, B.; Bourdot, P.; Bonnerot, J. M.

    2013-09-01

    The ECRIX-H experiment aims to assess the feasibility of transmuting americium micro-dispersed in an inert magnesia matrix under a locally moderated neutron flux in the Phénix reactor. A first set of examinations demonstrated that pellet behaviour was satisfactory with moderate swelling at the end of the irradiation. Additional post-irradiation examinations needed to be conducted to confirm the high transmutation rate so as to definitively conclude on the success of the ECRIX-H experiment. This article presents and discusses the results of these new examinations. They confirm the satisfactory behaviour of the MgO matrix not only during the basic irradiation but also during post-irradiation thermal transients. These examinations also provide additional information on the behaviour of fission products both in the americium-based particles and in the MgO matrix. These results particularly validate the transmutation rate predicted by the calculation codes using several different analytical techniques. The fission rate is also determined. Moderate pellet swelling under irradiation (6.7 vol.%), while only 23% of the produced He and 4% of the fission gases were released from the fuel. No interaction between the pellets and the cladding. Formation of bubbles due to the precipitation of fission gases and He mainly in bubbles located inside the americium-based particles. These bubbles are the main cause of macroscopic swelling in the pellets. Well-crystallised structure of the MgO matrix which shows no amorphisation after irradiation despite the presence of fission products. The absence of any reaction of MgO with the americium-based phase, Formation of a PuO2-type crystalline phase from AmO1.62 particles following the Am transmutation process. A shielded electron probe micro-analyser (EPMA) 'CAMECA' Camebax equipped to collect and exploit the measurements using the 'SAMx' system. A Philips XL30 scanning electron microscope (SEM). Field acquisitions were performed thanks to

  12. Americium and plutonium in water, biota, and sediment from the central Oregon coast

    SciTech Connect

    Nielsen, R. D.

    1982-06-01

    Plutonium-239, 240 and americium-241 were measured in the mussel Mytilus californianus from the region of Coos Bay, OR. The flesh of this species has a plutonium concentration of about 90 fCi/kg, and an Am-241/Pu-239, 240 ratio that is high relative to mixed fallout, ranging between two and three. Transuranic concentrations in sediment, unfiltered water, and filterable particulates were also measured; none of these materials has an Am/Pu ratio as greatly elevated as the mussels, and there is no apparent difference in the Am/Pu ratio of terrestrial runoff and coastal water. Sediment core profiles do not allow accumulation rates or depositional histories to be identified, but it does not appear that material characterized by a high Am/Pu ratio has ever been introduced to this estuary. Other bivalves (Tresus capax and Macoma nasuta) and a polychaete (Abarenicola sp.) do not have an elevated Am/Pu ratio, although the absolute activity of plutonium in the infaunal bivalves is roughly four times that in the mussels.

  13. Removal of plutonium and Americium from hydrochloric acid waste streams using extraction chromatography

    SciTech Connect

    Schulte, L.D.; FitzPatrick, J.R.; Salazar, R.R.; Schake, B.S.; Martinez, B.T.

    1995-01-01

    Extraction chromatography is under development as a method to lower actinide activity levels in hydrochloric acid (HCl) effluent streams. Successful application of this technique for radioactive liquid waste treatment would provide a low activity feedstream for HCl recycle, reduce the loss of radioactivity to the environment in aqueous effluents, and lower the quantity and improve the form of solid waste generated. The extraction of plutonium and americium from HCl solutions was examined for several commercial and laboratory-produced sorbed resin materials. Polymer beads were coated with n-octyl(phenyl)-N,N-diisobutylcarbamoyl- methylphosphine oxide (CMPO) and either tributyl phosphate (TBP), or diamyl amylphosphonate (DAAP). Distribution coefficients for Pu and Am were measured by contact studies in 1-10 M HCl, while varying REDOX conditions, actinide loading levels, and resin formulations. Flow experiments were run to evaluate actinide loading and elution under varied conditions. Significant differences in the actinide distribution coefficients in contact experiments, and in actinide retention in flow experiments were observed as a function of resin formulation.

  14. Preparation of curium-americium oxide microspheres by resin-bead loading

    SciTech Connect

    Chattin, F.R.; Benker, D.E.; Lloyd, M.H.; Orr, P.B.; Ross, R.G.; Wiggins, J.T.

    1980-01-01

    Resin-bead loading and calcination techniques have been used to produce all curium and americium oxide feed material (about 2.2 kg) for HFIR targets since 1971. The process based on Dowex 50W resin has progressed from a series of test runs, through special production runs, into routine production in permanent equipment beginning in 1975. Key attributes of this process are its reliability, high yields, and ease of operation. The process is suited for remote operation in hot cells. Yields approaching 95% are routinely obtained and only one unacceptable product has been generated during routine production operations. There have been no problems in fabricating targets from this oxide or in the subsequent irradiation of these targets. The present scale of production of 150 to 250 g/y supplies the present need and is comparable with the level of other chemical process operations at TRU. Since the annual production is accomplished in two 8 to 12 day periods, there has been no reason to consider further scale-up. However, the rate of production could easily be doubled by simply adding a second set of calcination equipment.

  15. Plutonium process control using an advanced on-line gamma monitor for uranium, plutonium, and americium

    SciTech Connect

    Marsh, S.F.; Miller, M.C.

    1987-05-01

    An on-line gamma monitor has been developed to profile uranium, plutonium, and americium in waste and product streams of the anion exchange process used to recover and purify plutonium at the Los Alamos Plutonium Facility. The gamma monitor employs passive gamma spectrometry to measure /sup 241/Am and /sup 239/Pu, based on their 59.5-keV and 129-keV gamma rays, respectively. Because natural and depleted uranium present in typical process streams have no gamma rays suitable for measurement by such passive methods, uranium measurement requires a novel and less direct technique. Plutonium-241, which is always present in plutonium processed at Los Alamos, decays primarily by beta emission to form /sup 241/Am. However, a small fraction of /sup 241/Pu decays by alpha emission to 6.8-day /sup 237/U. The short half-life and 208-keV gamma energy of /sup 237/U make it an ideal radiotracer to mark the position of macro amounts of uranium impurity in the separation process. The real-time data obtained from an operating process allow operators to optimize many process parameters. The gamma monitor also provides a permanent record of the daily performance of each ion exchange system. 2 refs., 12 figs.

  16. Development and Testing of an Americium/Lanthanide Separation Flowsheet Using Sodium Bismuthate

    SciTech Connect

    Jack Law; Bruce Mincher; Troy Garn; Mitchell Greenhalgh; Nicholas Schmitt; Veronica Rutledge

    2014-04-01

    The separation of Am from the lanthanides and curium is a key step in proposed advanced fuel cycle scenarios. The partitioning and transmutation of Am is desirable to minimize the long-term heat load of material interred in a future high-level waste repository. A separation process amenable to process scale-up remains elusive. Given only subtle chemistry differences within and between the ions of the trivalent actinide and lanthanide series this separation is challenging ; however, higher oxidation states of americium can be prepared using sodium bismuthate and separated via solvent extraction using diamylamylphosphonate (DAAP) extraction. Among the other trivalent metals only Ce is also oxidized and extracted. Due to the long-term instability of Am(VI) , the loaded organic phase is readily selectively stripped to partition the actinide to a new acidic aqueous phase. Batch extraction distribution ratio measurements were used to design a flowsheet to accomplish this separation. Additionally, crossflow filtration was investigated as a method to filter the bismuthate solids from the feed solution prior to extraction. Results of the filtration studies, flowsheet development work and flowsheet performance testing using a centrifugal contactor are detailed.

  17. Americium-based oxides: Dense pellet fabrication from co-converted oxalates

    NASA Astrophysics Data System (ADS)

    Horlait, Denis; Lebreton, Florent; Gauthé, Aurélie; Caisso, Marie; Arab-Chapelet, Bénédicte; Picart, Sébastien; Delahaye, Thibaud

    2014-01-01

    Mixed oxides are used as nuclear fuels and are notably envisaged for future fuel cycles including plutonium and minor actinide recycling. In this context, processes are being developed for the fabrication of uranium-americium mixed-oxide compounds for transmutation. The purpose of these processes is not only the compliance with fuel specifications in terms of density and homogeneity, but also the simplification of the process for its industrialization as well as lowering dust generation. In this paper, the use of a U0.85Am0.15O2±δ powder synthesized by oxalate co-conversion as a precursor for dense fuel fabrications is assessed. This study notably focuses on sintering, which yielded pellets up to 96% of the theoretical density, taking advantage of the high reactivity and homogeneity of the powder. As-obtained pellets were further characterized to be compared to those obtained via processes based on the UMACS (Uranium Minor Actinide Conventional Sintering) process. This comparison highlights several advantages of co-converted powder as a precursor for simplified processes that generate little dust.

  18. Solution speciation of plutonium and Americium at an Australian legacy radioactive waste disposal site.

    PubMed

    Ikeda-Ohno, Atsushi; Harrison, Jennifer J; Thiruvoth, Sangeeth; Wilsher, Kerry; Wong, Henri K Y; Johansen, Mathew P; Waite, T David; Payne, Timothy E

    2014-09-01

    During the 1960s, radioactive waste containing small amounts of plutonium (Pu) and americium (Am) was disposed in shallow trenches at the Little Forest Burial Ground (LFBG), located near the southern suburbs of Sydney, Australia. Because of periodic saturation and overflowing of the former disposal trenches, Pu and Am have been transferred from the buried wastes into the surrounding surface soils. The presence of readily detected amounts of Pu and Am in the trench waters provides a unique opportunity to study their aqueous speciation under environmentally relevant conditions. This study aims to comprehensively investigate the chemical speciation of Pu and Am in the trench water by combining fluoride coprecipitation, solvent extraction, particle size fractionation, and thermochemical modeling. The predominant oxidation states of dissolved Pu and Am species were found to be Pu(IV) and Am(III), and large proportions of both actinides (Pu, 97.7%; Am, 86.8%) were associated with mobile colloids in the submicron size range. On the basis of this information, possible management options are assessed. PMID:25126837

  19. Americium characterization by X-ray fluorescence and absorption spectroscopy in plutonium uranium mixed oxide

    NASA Astrophysics Data System (ADS)

    Degueldre, Claude; Cozzo, Cedric; Martin, Matthias; Grolimund, Daniel; Mieszczynski, Cyprian

    2013-06-01

    Plutonium uranium mixed oxide (MOX) fuels are currently used in nuclear reactors. The actinides in these fuels need to be analyzed after irradiation for assessing their behaviour with regard to their environment and the coolant. In this work the study of the atomic structure and next-neighbour environment of Am in the (Pu,U)O2 lattice in an irradiated (60 MW d kg-1) MOX sample was performed employing micro-X-ray fluorescence (µ-XRF) and micro-X-ray absorption fine structure (µ-XAFS) spectroscopy. The chemical bonds, valences and stoichiometry of Am (˜0.66 wt%) are determined from the experimental data gained for the irradiated fuel material examined in its peripheral zone (rim) of the fuel. In the irradiated sample Am builds up as Am3+ species within an [AmO8]13- coordination environment (e.g. >90%) and no (<10%) Am(IV) or (V) can be detected in the rim zone. The occurrence of americium dioxide is avoided by the redox buffering activity of the uranium dioxide matrix.

  20. Characterization of neutron calibration fields at the TINT's 50 Ci americium-241/beryllium neutron irradiator

    NASA Astrophysics Data System (ADS)

    Liamsuwan, T.; Channuie, J.; Ratanatongchai, W.

    2015-05-01

    Reliable measurement of neutron radiation is important for monitoring and protection in workplace where neutrons are present. Although Thailand has been familiar with applications of neutron sources and neutron beams for many decades, there is no calibration facility dedicated to neutron measuring devices available in the country. Recently, Thailand Institute of Nuclear Technology (TINT) has set up a multi-purpose irradiation facility equipped with a 50 Ci americium-241/beryllium neutron irradiator. The facility is planned to be used for research, nuclear analytical techniques and, among other applications, calibration of neutron measuring devices. In this work, the neutron calibration fields were investigated in terms of neutron energy spectra and dose equivalent rates using Monte Carlo simulations, an in-house developed neutron spectrometer and commercial survey meters. The characterized neutron fields can generate neutron dose equivalent rates ranging from 156 μSv/h to 3.5 mSv/h with nearly 100% of dose contributed by neutrons of energies larger than 0.01 MeV. The gamma contamination was less than 4.2-7.5% depending on the irradiation configuration. It is possible to use the described neutron fields for calibration test and routine quality assurance of neutron dose rate meters and passive dosemeters commonly used in radiation protection dosimetry.

  1. Plutonium and americium recovery from spent molten-salt-extraction salts with aluminum-magnesium alloys

    SciTech Connect

    Cusick, M.J.; Sherwood, W.G.; Fitzpatrick, R.F.

    1984-04-23

    Development work was performed to determine the feasibility of removing plutonium and americium from spent molten-salt-extraction (MSE) salts using Al-Mg alloys. If the product buttons from this process are compatible with subsequent aqueous processing, the complex chloride-to-nitrate aqueous conversion step which is presently required for these salts may be eliminated. The optimum alloy composition used to treat spent 8 wt % MSE salts in the past yielded poor phase-disengagement characteristics when applied to 30 mol % salts. After a limited investigation of other alloy compositions in the Al-Mg-Pu-Am system, it was determined that the Al-Pu-Am system could yield a compatible alloy. In this system, experiments were performed to investigate the effects of plutonium loading in the alloy, excess magnesium, age of the spent salt on actinide recovery, phase disengagement, and button homogeneity. Experimental results indicate that 95 percent plutonium recoveries can be attained for fresh salts. Further development is required for backlog salts generated prior to 1981. A homogeneous product alloy, as required for aqueous processing, could not be produced.

  2. Osteosarcoma development following single inhalation exposure to americium-241 in beagle dogs

    SciTech Connect

    Gillett, N.A.; Hahn, F.F.; Mewhinney, J.A.; Muggenberg, B.A.

    1985-10-01

    Young, mature Beagle dogs underwent single inhalation exposure to respirable aerosols of SU AmO2 to determine the radiation dose distribution to tissues. The dogs were serially sacrificed to assess the clearance of SU Am from the lung, the rate of translocation to internal organs, the pattern of retention in the organs, and the rates and modes of excretion. Americium dioxide was relatively soluble in the lung, leading to the translocation of significant quantities of SU Am to bone and liver, thus delivering radiation doses to these tissues nearly equal to that received by the lung. Osteoblastic osteosarcomas developed in four dogs surviving more than 1000 days after exposure. Histologically, all of the osteosarcomas were associated with areas of radiation osteodystrophy characterized by bone infarction, peritrabecular new bone formation, marrow fibrosis, and microresorptive cavities. The retention and translocation of inhaled SU Am in dogs is similar to that of man, indicating that 241Am inhaled by humans may potentially result in significant risk of bone tumor development.

  3. Assessment of radiation doses from residential smoke detectors that contain americium-241

    SciTech Connect

    O'Donnell, F.R.; Etnier, E.L.; Holton, G.A.; Travis, C.C.

    1981-10-01

    External dose equivalents and internal dose commitments were estimated for individuals and populations from annual distribution, use, and disposal of 10 million ionization chamber smoke detectors that contain 110 kBq (3 ..mu..Ci) americium-241 each. Under exposure scenarios developed for normal distribution, use, and disposal using the best available information, annual external dose equivalents to average individuals were estimated to range from 4 fSv (0.4 prem) to 20 nSv (2 ..mu..rem) for total body and from 7 fSv to 40 nSv for bone. Internal dose commitments to individuals under post disposal scenarios were estimated to range from 0.006 to 80 ..mu..Sv (0.0006 to 8 mrem) to total body and from 0.06 to 800 ..mu..Sv to bone. The total collective dose (the sum of external dose equivalents and 50-year internal dose commitments) for all individuals involved with distribution, use, or disposal of 10 million smoke detectors was estimated to be about 0.38 person-Sv (38 person-rem) to total body and 00 ft/sup 2/).

  4. In Vitro Dissolution Tests of Plutonium and Americium Containing Contamination Originating From ZPPR Fuel Plates

    SciTech Connect

    William F. Bauer; Brian K. Schuetz; Gary M. Huestis; Thomas B. Lints; Brian K. Harris; R. Duane Ball; Gracy Elias

    2012-09-01

    Assessing the extent of internal dose is of concern whenever workers are exposed to airborne radionuclides or other contaminants. Internal dose determinations depend upon a reasonable estimate of the expected biological half-life of the contaminants in the respiratory tract. One issue with refractory elements is determining the dissolution rate of the element. Actinides such as plutonium (Pu) and Americium (Am) tend to be very refractory and can have biological half-lives of tens of years. In the event of an exposure, the dissolution rates of the radionuclides of interest needs to be assessed in order to assign the proper internal dose estimates. During the November 2011 incident at the Idaho National Laboratory (INL) involving a ZPPR fuel plate, air filters in a constant air monitor (CAM) and a giraffe filter apparatus captured airborne particulate matter. These filters were used in dissolution rate experiments to determine the apparent dissolution half-life of Pu and Am in simulated biological fluids. This report describes these experiments and the results. The dissolution rates were found to follow a three term exponential decay equation. Differences were noted depending upon the nature of the biological fluid simulant. Overall, greater than 95% of the Pu and 93% of the Am were in a very slow dissolving component with dissolution half-lives of over 10 years.

  5. ISOTOPE SEPARATORS

    DOEpatents

    Bacon, C.G.

    1958-08-26

    An improvement is presented in the structure of an isotope separation apparatus and, in particular, is concerned with a magnetically operated shutter associated with a window which is provided for the purpose of enabling the operator to view the processes going on within the interior of the apparatus. The shutier is mounted to close under the force of gravity in the absence of any other force. By closing an electrical circuit to a coil mouated on the shutter the magnetic field of the isotope separating apparatus coacts with the magnetic field of the coil to force the shutter to the open position.

  6. Use of EIChroM TRU RESIN in the determination of Americium, Plutonium and Uranium in air filter and water samples

    SciTech Connect

    Berne, Anna

    1995-03-01

    TRU Resin, an extraction chromatographic material ((octyl (phenyl)-N,Ndiisobutylcarbamoylmethylphosphene oxide (CMPO) dissolved in tributyl phosphate (TBP)) manufactured by EIChroM Industries, was tested for its actinide sorption and desorption characteristics. A study was initiated to demonstrate the effectiveness of extracting plutonium, americium and uranium from water and air filter samples from the Environmental Measurements Laboratory’s Quality Assessment Program (QAP), and the effectiveness of subsequent desorption of one chemical species at a time in order to prepare each of them for spectrometry. Crossover of plutonium into the americium fraction with the TRU Resin was observed and could not be eliminated while using TRU Resin only. However, prior extraction of plutonium using an anion exchange resin can overcome this problem. A method for the determination of americium is proposed which combines the extraction of plutonium onto Bio-Rad AG 1-X8 anion exchange resin with the extraction of americium using the TRU Resin. This method was tested on three triplicate sets of QAP air filters and two triplicate sets of QAP water samples. The recoveries ranged from 70 to 90 percent, and the results were identical to those obtained by the existing methods. The time required to perform the analysis for americium was shortened from 5 weeks to 1 week.

  7. Use of EIChroM`s TRU resin in the determination of americium, plutonium and uranium in air filter and water samples

    SciTech Connect

    Berne, A.

    1995-12-01

    TRU Resin, an extraction chromatographic material (octyl (phenyl)-N,Ndiisobutylcarbamoyl-methylphosphene oxide (CMPO) dissolved in tributyl phosphate (TBP)) manufactured by EIChroM Industries, was tested for its actinide sorption and desorption characteristics. A study was initiated to demonstrate the effectiveness of extracting plutonium, americium and uranium from water and air filter samples from the Environmental Measurements Laboratory`s Quality Assessment Program (QAP), and the effectiveness of subsequent desorption of one chemical species at a time in order to prepare each of them for a spectrometry. Crossover of plutonium into the americium fraction with the TRU Resin was observed and could not be eliminated while using TRU Resin only. However, prior extraction of plutonium using an anion exchange resin can overcome this problem. A method for the determination of americium is proposed which combines the extraction of plutonium onto Bio-Rad AG 1-X8 anion exchange resin with the extraction of americium using the TRU Resin. This method was tested on three triplicate sets of QAP air filters and two triplicate sets of QAP water samples. The recoveries ranged from 70 to 90 percent, and the results were identical to those obtained by the existing methods. The time required to perform the analysis for americium was shortened from 5 weeks to 1 week.

  8. Americium-Curium Stabilization - 5'' Cylindrical Induction Melter System Design Basis

    SciTech Connect

    Witt, D.C.

    1999-11-08

    Approximately 11,000 liters (3,600) gallons of solution containing isotopes of Am and Cm are currently stored in F-Canyon Tank 17.1. These isotopes were recovered during plutonium-242 production campaigns in the mid- and late-1970s. Experimental work for the project began in 1995 by the Savannah River Technology Center (SRTC). Details of the process are given in the various sections of this document.

  9. Adsorption and dissociation of molecular hydrogen on the (0001) surface of double hexagonal close packed americium

    NASA Astrophysics Data System (ADS)

    Dholabhai, P. P.; Ray, A. K.

    2009-01-01

    Hydrogen molecule adsorption on the (0001) surface of double hexagonal packed americium has been studied in detail within the framework of density functional theory using a full-potential all-electron linearized augmented plane wave plus local orbitals method (FP-L/APW+lo). Weak molecular hydrogen adsorptions were observed. Adsorption energies were optimized with respect to the distance of the adsorbates from the surface for three approach positions at three adsorption sites, namely t1 (one-fold top), b2 (two-fold bridge), and h3 (three-fold hollow) sites. Adsorption energies were computed at the scalar-relativistic level (no spin-orbit coupling NSOC) and at the fully relativistic level (with spin-orbit coupling SOC). The most stable configuration corresponds to a horizontal adsorption with the molecular approach being perpendicular to a lattice vector. The surface coverage is equivalent to one-fourth of a monolayer (ML), with the adsorption energies at the NSOC and SOC theoretical levels being 0.0997 eV and 0.1022 eV, respectively. The respective distance of the hydrogen molecule from the surface and hydrogen-hydrogen distance was found to be 2.645 Å and 0.789 Å, respectively. The work functions decreased and the net magnetic moments remained almost unchanged in all cases compared with the corresponding quantities of bare dhcp Am (0001) surface. The adsorbate-substrate interactions have been analyzed in detail using the partial charges inside the muffin-tin spheres, difference charge density distributions, and the local density of states. The effects of adsorption on the Am 5f electron localization-delocalization characteristics have been discussed. Reaction barrier for the dissociation of hydrogen molecule has been presented.

  10. Investigation of the neutron spectrum of americium-beryllium sources by Bonner sphere spectrometry

    NASA Astrophysics Data System (ADS)

    Bedogni, R.; Domingo, C.; Roberts, N.; Thomas, D. J.; Chiti, M.; Esposito, A.; Garcia, M. J.; Gentile, A.; Liu, Z. Z.; de-San-Pedro, M.

    2014-11-01

    Americium-beryllium neutron sources are certainly the most widely used in neutron dosimetry laboratories, basically due to their long half-life and their energy distribution, which covers the energy domain of interest for many applications in ambient and personal dosimetry. Nevertheless, the spectrum of this source depends on the materials and dimension of the capsule and on the amount and physical-chemical properties of the active material, thus affecting relevant quantities such as the spectrum-averaged fluence-to-dose equivalent conversion coefficient. A EURAMET (European Association of National Metrology Institutes) project (n. 1104) was initiated to experimentally investigate how the neutron spectrum changes for different source sizes and encapsulations with a view to providing improved data for a planned revision of the ISO 8529 Standard Series. The experimental campaign was carried out in the low scatter facility at NPL. Here three different Bonner sphere spectrometers, BSSs, were exposed to the neutron fields produced by three different neutron sources formats: one X3 capsule (1 Ci) and two X14 capsules (10 Ci and 15 Ci). The specific advantage of the BSS is the large sensitivity to low-energy neutrons (E<0.1 MeV) which is the component expected to be most affected by the capsule-to-capsule variations and the component which is least well known. This paper summarises the results of the campaign with emphasis on (1) estimating the low-energy component of the Am-Be neutron spectrum, according to the encapsulation type; (2) evaluating the coherence between the Bonner spheres data and the previous studies performed with high-resolution spectrometers but limited in energy to E>0.1 MeV; (3) understanding whether the ISO-recommended Am-Be spectrum needs to be amended, and for which source formats.

  11. Americium and plutonium association with magnesium hydroxide colloids in alkaline nuclear industry process environments

    NASA Astrophysics Data System (ADS)

    Maher, Zoe; Ivanov, Peter; O'Brien, Luke; Sims, Howard; Taylor, Robin J.; Heath, Sarah L.; Livens, Francis R.; Goddard, David; Kellet, Simon; Rand, Peter; Bryan, Nick D.

    2016-01-01

    The behaviours of Pu, Am and colloids in feed solutions to the Site Ion-exchange Effluent Plant (SIXEP) at the Sellafield nuclear reprocessing site in the U.K. have been studied. For both Pu and Am, fractions were found to be associated with material in the colloidal size range, with ˜50% of the Pu in the range 1-200 nm. The concentration of soluble Pu (<1 nm) was ˜1 nM, which is very similar to the solubility limit for Pu(V). The soluble Am concentration was of the order of 10-11 M, which was below the solubility limit of americium hydroxide. The size, morphology and elemental composition of the particulates and colloids in the feed solutions were investigated. Magnesium is homogeneously distributed throughout the particles, whereas U, Si, Fe, and Ca were present in localised areas only. Amongst some heterogeneous material, particles were identified that were consistent with hydrotalcite. The distribution of 241Am(III) on brucite (magnesium hydroxide) colloids of different sizes was studied under alkaline conditions representative of nuclear fuel storage pond and effluent feed solution conditions. The morphology of the brucite particles in the bulk material observed by ESEM was predominantly hexagonal, while that of the carbonated brucite consisted of hexagonal species mixed with platelets. The association of 241Am(III) with the brucite colloids was studied by ultrafiltration coupled with gamma ray-spectrometry. For carbonate concentrations up to 10-3 M, the 241Am(III) was mainly associated with larger colloids (>300 kDa), and there was a shift from the smaller size fractions to the larger over a period of 6 months. At higher carbonate concentrations (10-2 M), the Am was predominantly detected in the true solution fraction (<3 kDa) and in smaller size colloidal fractions, in the range 3-100 kDa.

  12. Americium/Lanthanide Separations in Alkaline Solutions for Advanced Nuclear Fuel Cycles

    SciTech Connect

    Goff, George S.; Long, Kristy Marie; Reilly, Sean D.; Jarvinen, Gordon D.; Runde, Wolfgang H.

    2012-06-11

    Project goals: Can used nuclear fuel be partitioned by dissolution in alkaline aqueous solution to give a solution of uranium, neptunium, plutonium, americium and curium and a filterable solid containing nearly all of the lanthanide fission products and certain other fission products? What is the chemistry of Am/Cm/Ln in oxidative carbonate solutions? Can higher oxidation states of Am be stabilized and exploited? Conclusions: Am(VI) is kinetically stable in 0.5-2.0 M carbonate solutions for hours. Aliquat 336 in toluene has been successfully shown to extract U(VI) and Pu(VI) from carbonate solutions. (Stepanov et al 2011). Higher carbonate concentration gives lower D, SF{sub U/Eu} for = 4 in 1 M K{sub 2}CO{sub 3}. Experiments with Am(VI) were unsuccessful due to reduction by the organics. Multiple sources of reducing organics...more optimization. Reduction experiments of Am(VI) in dodecane/octanol/Aliquat 336 show that after 5 minutes of contact, only 30-40% of the Am(VI) has been reduced. Long enough to perform an extraction. Shorter contact times, lower T, and lower Aliquat 336 concentration still did not result in any significant extraction of Am. Anion exchange experiments using a strong base anion exchanger show uptake of U(VI) with minimal uptake of Nd(III). Experiments with Am(VI) indicate Am sorption with a Kd of 9 (10 minute contact) but sorption mechanism is not yet understood. SF{sub U/Nd} for = 7 and SF{sub U/Eu} for = 19 after 24 hours in 1 M K{sub 2}CO{sub 3}.

  13. EFFECT OF COMPOSITION OF SELECTED GROUNDWATERS FROM THE BASIN AND RANGE PROVINCE ON PLUTONIUM, NEPTUNIUM, AND AMERICIUM SPECIATION.

    USGS Publications Warehouse

    Rees, Terry F.; Cleveland, Jess M.; Nash, Kenneth L.

    1984-01-01

    The speciation of plutonium, neptunium, and americium was determined in groundwaters from four sources in the Basin and Range Province: the lower carbonate aquifer, Nevada Test Site (NTS) (Crystal Pool); alluvial fill, Frenchman Flat, NTS (well 5C); Hualapai Valley, Arizona (Red Lake south well); and Tularosa Basin, New Mexico (Rentfrow well). The results were interpreted to indicate that plutonium and, to a lesser extent, neptunium are least soluble in reducing groundwaters containing a large concentration of sulfate ion and a small concentration of strongly complexing anions. The results further emphasize the desirability of including studies such as this among the other site-selection criteria for nuclear waste repositories.

  14. The solvent extraction of americium(III) in HCl solutions by 2,6-bis[(diphenylphospino)methyl]pyridine N,P,P{prime}-trioxide

    SciTech Connect

    Bond, E.M.; Engelhardt, U.; Deere, T.P.; Rapko, B.M.; Paine, R.T.; FitzPatrick, J.R.

    1998-07-01

    The liquid/liquid extraction of Am(III) from hydrochloric acid solutions with chloroform solutions of 2,6-bis[(diphenylphosphino)methyl]pyridine N,P,P{prime}-trioxide (ENOPOPO) is described. ENOPOPO exhibits modest extraction ability for americium(III) (D{sub Am} = 2.2 at 5 M HCl) and can be efficiently back extracted from the organic phase at 0.1 M HCl. The ligand dependency data suggest that three ligand molecules are coordinated to the americium in the extraction complex. Additional aspects of the extraction mechanism are described.

  15. Swelling under irradiation of MgO pellets containing americium oxide: The ECRIX-H irradiation experiment

    NASA Astrophysics Data System (ADS)

    Lamontagne, J.; Béjaoui, S.; Hanifi, K.; Valot, Ch.; Loubet, L.

    2011-06-01

    The ECRIX-H irradiation experiment studied the behaviour of pellets containing americium dispersed in MgO. The purpose of the irradiation was to demonstrate the capacity of magnesia to provide an efficient support matrix. After fabrication, the sintered pellets contained 16.65 wt.% of Am microdispersed in the inert matrix. The ECRIX-H pellets were irradiated under a locally moderated neutron flux in the Phénix sodium-cooled fast reactor (SFR) for 318 Effective Full Power Days (EFPD). Post-test calculations indicated that the fission and transmutation rates of americium at the maximum flux plane reached 33.9% and 92.6% respectively at the end of the irradiation phase. The results of the post-irradiation examinations - both non-destructive and destructive - are discussed in this paper. These results indicate a satisfactory behaviour of the MgO matrix. Particularly, a moderate swelling occurs in the pellets under irradiation even with significant quantities of helium generated and at high transmutation rate.

  16. Temperature and concentration dependences of the electrical resistivity for alloys of plutonium with americium under normal conditions

    SciTech Connect

    Tsiovkin, Yu. Yu. Povzner, A. A.; Tsiovkina, L. Yu.; Dremov, V. V.; Kabirova, L. R.; Dyachenko, A. A.; Bystrushkin, V. B.; Ryabukhina, M. V.; Lukoyanov, A. V.; Shorikov, A. O.

    2010-01-15

    The temperature and concentration dependences of the electrical resistivity for alloys of americium with plutonium are analyzed in terms of the multiband conductivity model for binary disordered substitution-type alloys. For the case of high temperatures (T > {Theta}{sub D}, {Theta}{sub D} is the Debye temperature), a system of self-consistent equations of the coherent potential approximation has been derived for the scattering of conduction electrons by impurities and phonons without any constraints on the interaction intensity. The definitions of the shift and broadening operator for a single-electron level are used to show qualitatively and quantitatively that the pattern of the temperature dependence of the electrical resistivity for alloys is determined by the balance between the coherent and incoherent contributions to the electron-phonon scattering and that the interference conduction electron scattering mechanism can be the main cause of the negative temperature coefficient of resistivity observed in some alloys involving actinides. It is shown that the great values of the observed resistivity may be attributable to interband transitions of charge carriers and renormalization of their effective mass through strong s-d band hybridization. The concentration and temperature dependences of the resistivity for alloys of plutonium and americium calculated in terms of the derived conductivity model are compared with the available experimental data.

  17. Preconcentration of low levels of americium and plutonium from waste waters by synthetic water-soluble metal-binding polymers with ultrafiltration

    SciTech Connect

    Smith, B.F.; Gibson, R.R.; Jarvinen, G.D.; Robison, T.W.; Schroeder, N.C.; Stalnaker, N.D.

    1997-12-31

    A preconcentration approach to assist in the measurement of low levels of americium and plutonium in waste waters has been developed based on the concept of using water-soluble metal-binding polymers in combination with ultrafiltration. The method has been optimized to give over 90% recovery and accountability from actual waste water.

  18. In situ characterization of uranium and americium oxide solid solution formation for CRMP process: first combination of in situ XRD and XANES measurements.

    PubMed

    Caisso, Marie; Picart, Sébastien; Belin, Renaud C; Lebreton, Florent; Martin, Philippe M; Dardenne, Kathy; Rothe, Jörg; Neuville, Daniel R; Delahaye, Thibaud; Ayral, André

    2015-04-14

    Transmutation of americium in heterogeneous mode through the use of U1-xAmxO2±δ ceramic pellets, also known as Americium Bearing Blankets (AmBB), has become a major research axis. Nevertheless, in order to consider future large-scale deployment, the processes involved in AmBB fabrication have to minimize fine particle dissemination, due to the presence of americium, which considerably increases the risk of contamination. New synthesis routes avoiding the use of pulverulent precursors are thus currently under development, such as the Calcined Resin Microsphere Pelletization (CRMP) process. It is based on the use of weak-acid resin (WAR) microspheres as precursors, loaded with actinide cations. After two specific calcinations under controlled atmospheres, resin microspheres are converted into oxide microspheres composed of a monophasic U1-xAmxO2±δ phase. Understanding the different mechanisms during thermal conversion, that lead to the release of organic matter and the formation of a solid solution, appear essential. By combining in situ techniques such as XRD and XAS, it has become possible to identify the key temperatures for oxide formation, and the corresponding oxidation states taken by uranium and americium during mineralization. This paper thus presents the first results on the mineralization of (U,Am) loaded resin microspheres into a solid solution, through in situ XAS analysis correlated with HT-XRD. PMID:25742991

  19. LIBS Spectral Data for a Mixed Actinide Fuel Pellet Containing Uranium, Plutonium, Neptunium and Americium

    SciTech Connect

    Judge, Elizabeth J.; Berg, John M.; Le, Loan A.; Lopez, Leon N.; Barefield, James E.

    2012-06-18

    Laser-induced breakdown spectroscopy (LIBS) was used to analyze a mixed actinide fuel pellet containing 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2}. The preliminary data shown here is the first report of LIBS analysis of a mixed actinide fuel pellet, to the authors knowledge. The LIBS spectral data was acquired in a plutonium facility at Los Alamos National Laboratory where the sample was contained within a glove box. The initial installation of the glove box was not intended for complete ultraviolet (UV), visible (VIS) and near infrared (NIR) transmission, therefore the LIBS spectrum is truncated in the UV and NIR regions due to the optical transmission of the window port and filters that were installed. The optical collection of the emission from the LIBS plasma will be optimized in the future. However, the preliminary LIBS data acquired is worth reporting due to the uniqueness of the sample and spectral data. The analysis of several actinides in the presence of each other is an important feature of this analysis since traditional methods must chemically separate uranium, plutonium, neptunium, and americium prior to analysis. Due to the historic nature of the sample fuel pellet analyzed, the provided sample composition of 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2} cannot be confirm without further analytical processing. Uranium, plutonium, and americium emission lines were abundant and easily assigned while neptunium was more difficult to identify. There may be several reasons for this observation, other than knowing the exact sample composition of the fuel pellet. First, the atomic emission wavelength resources for neptunium are limited and such techniques as hollow cathode discharge lamp have different dynamics than the plasma used in LIBS which results in different emission spectra. Secondly, due to the complex sample of four actinide elements, which all have very dense electronic energy levels, there may be reactions and

  20. Peculiar Behavior of (U,Am)O(2-δ) Compounds for High Americium Contents Evidenced by XRD, XAS, and Raman Spectroscopy.

    PubMed

    Lebreton, Florent; Horlait, Denis; Caraballo, Richard; Martin, Philippe M; Scheinost, Andreas C; Rossberg, Andre; Jégou, Christophe; Delahaye, Thibaud

    2015-10-19

    In U(1-x)Am(x)O(2±δ) compounds with low americium content (x ≤ 20 atom %) and oxygen-to-metal (O/M) ratios close to 2.0, Am(III+) cations are charge-balanced by an equivalent amount of U(V+) cations while the fluorite structure of pure U(IV+)O2 is maintained. Up to now, it is unknown whether this observation also holds for higher americium contents. In this study, we combined X-ray diffraction with Raman and X-ray absorption spectroscopies to investigate a U(0.5)Am(0.5)O(2±δ) compound. Our results indicate that americium is again only present as Am(III+), while U(V+) remains below the amount required for charge balance. Unlike lower americium contents, this leads to an overall oxygen hypostoichiometry with an average O/M ratio of 1.92(2). The cationic sublattice is only slightly affected by the coexistence of large amounts of reduced (Am(III+)) and oxidized (U(V+)) cations, whereas significant deviations from the fluorite structure are evidenced by both extended X-ray absorption fine structure and Raman spectroscopies in the oxygen sublattice, with the observation of both vacancies and interstitials, the latter being apparently consistent with the insertion of U6O12 cuboctahedral-type clusters (as observed in the U4O9 or U3O7 phases). These results thus highlight the specificities of uranium-americium mixed oxides, which behave more like trivalent lanthanide-doped UO2 than U(1-x)Pu(x)O(2±δ) MOX fuels. PMID:26407031

  1. Novel Americium Treatment Process for Surface Water and Dust Suppression Water

    SciTech Connect

    Tiepel, E.W.; Pigeon, P.; Nesta, S.; Anderson, J.

    2006-07-01

    The Rocky Flats Environmental Technology Site (RFETS), a former nuclear weapons production plant, has been remediated under CERCLA and decommissioned to become a National Wildlife Refuge. The site conducted this cleanup effort under the Rocky Flats Cleanup Agreement (RFCA) that established limits for the discharge of surface and process waters from the site. At the end of 2004, while a number of process buildings were undergoing decommissioning, routine monitoring of a discharge pond (Pond A-4) containing approximately 28 million gallons of water was discovered to have been contaminated with a trace amount of Americium-241 (Am-241). While the amount of Am-241 in the pond waters was very low (0.5 - 0.7 pCi/l), it was above the established Colorado stream standard of 0.15 pCi/l for release to off site drainage waters. The rapid successful treatment of these waters to the regulatory limit was important to the site for two reasons. The first was that the pond was approaching its hold-up limit. Without rapid treatment and release of the Pond A-4 water, typical spring run-off would require water management actions to other drainages onsite or a mass shuttling of water for disposal. The second reason was that this type of contaminated water had not been treated to the stringent stream standard at Rocky Flats before. Technical challenges in treatment could translate to impacts on water and secondary waste management, and ultimately, cost impacts. All of the technical challenges and specific site criteria led to the conclusion that a different approach to the treatment of this problem was necessary and a crash treatability program to identify applicable treatment techniques was undertaken. The goal of this program was to develop treatment options that could be implemented very quickly and would result in the generation of no high volume secondary waste that would be costly to dispose. A novel chemical treatment system was developed and implemented at the RFETS to treat Am

  2. Thermodynamic Features of the Complexation of Neodymium(III) and Americium(III) by Lactate in Trifluoromethanesulfonate Media.

    SciTech Connect

    Peter R. Zalupski; Leigh R. Martin; Kenneth L. Nash

    2010-10-01

    The protonation of lactate has been studied in a variety of electrolyte solutions using microcalorimetry to reveal a distinct medium influence imposed on the thermochemistry of the investigated equilibrium. The thermochemistry of lactate protonation, when studied directly in 1.0 M sodium lactate, agreed well with the studies performed in trifluoromethanesulfonate (triflate). This thermodynamic agreement suggests that the physical chemistry of lactate in the solutions applicable to the TALSPEAK process – a solvent extraction method for separating trivalent actinides from trivalent lanthanides within the scope of used nuclear fuel processing efforts – may be simulated in triflate solutions. Potentiometry, spectrophotometry and microcalorimetry have been subsequently used to study the thermodynamic features of neodymium and americium complexation by lactate using triflate as a strong background electrolyte. Three successive mononuclear lactate complexes were identified for Nd(III) and Am(III). The stability constants for neodymium, log ß1 = 2.60 ± 0.01, log ß2 = 4.66 ± 0.02 and log ß3 = 5.6 ± 0.1, and for americium, log ß1 = 2.60 ± 0.06, log ß2 = 4.7 ± 0.1 and log ß3 = 6.2 ± 0.2, were found to closely agree with the thermodynamic studies reported in sodium perchlorate solutions. Consequently, the thermodynamic medium effect, imposed on the TALSPEAK-related solution equilibria by the presence of strong background electrolytes such as NaClO4 and NaNO3, do not significantly impact the speciation in solution.

  3. Method for separating isotopes

    DOEpatents

    Jepson, B.E.

    1975-10-21

    Isotopes are separated by contacting a feed solution containing the isotopes with a cyclic polyether wherein a complex of one isotope is formed with the cyclic polyether, the cyclic polyether complex is extracted from the feed solution, and the isotope is thereafter separated from the cyclic polyether.

  4. Stable isotope studies

    SciTech Connect

    Ishida, T.

    1992-01-01

    The research has been in four general areas: (1) correlation of isotope effects with molecular forces and molecular structures, (2) correlation of zero-point energy and its isotope effects with molecular structure and molecular forces, (3) vapor pressure isotope effects, and (4) fractionation of stable isotopes. 73 refs, 38 figs, 29 tabs.

  5. Impact of environmental curium on plutonium migration and isotopic signatures.

    PubMed

    Kurosaki, Hiromu; Kaplan, Daniel I; Clark, Sue B

    2014-12-01

    Plutonium (Pu), americium (Am), and curium (Cm) activities were measured in sediments from a former radioactive waste disposal basin located on the Savannah River Site, South Carolina, and in subsurface aquifer sediments collected downgradient from the basin. In situ Kd values (Pu concentration ratio of sediment/groundwater) derived from this field data and previously reported groundwater concentration data compared well to laboratory Kd values reported in the literature. Pu isotopic signatures confirmed multiple sources of Pu contamination. The ratio of (240)Pu/(239)Pu was appreciably lower for sediment samples compared to the associated groundwater. This isotopic ratio difference may be explained by the following: (1) (240)Pu produced by decay of (244)Cm may exist predominantly in high oxidation states (Pu(V)O2(+) and Pu(VI)O2(2+)) compared to Pu derived from the disposed waste effluents, and (2) oxidized forms of Pu sorb less to sediments than reduced forms of Pu. Isotope-specific Kd values calculated from measured Pu activities in the sediments and groundwater indicated that (240)Pu, which is derived primarily from the decay of (244)Cm, had a value of 10 ± 2 mL g(-1), whereas (239)Pu originating from the waste effluents discharged at the site had a value of 101 ± 8 mL g(-1). One possible explanation for the isotope-specific sorption behavior is that (240)Pu likely existed in the weaker sorbing oxidation states, +5 or +6, than (239)Pu, which likely existed in the +3 or +4 oxidation states. Consequently, remediation strategies for radioactively contaminated systems must consider not only the discharged contaminants but also their decay products. In this case, mitigation of Cm as well as Pu will be required to completely address Pu migration from the source term. PMID:25350948

  6. Americium and plutonium separation by extraction chromatography for determination by accelerator mass spectrometry.

    PubMed

    Kazi, Zakir H; Cornett, Jack R; Zhao, Xaiolei; Kieser, Liam

    2014-06-01

    A simple method was developed to separate Pu and Am using single column extraction chromatography employing N,N,N',N'-tetra-n-octyldiglycolamide (DGA) resin. Isotope dilution measurements of Am and Pu were performed using accelerator mass spectrometry (AMS) and alpha spectrometry. For maximum adsorption Pu was stabilized in the tetra valent oxidation state in 8M HNO3 with 0.05 M NaNO2 before loading the sample onto the resin. Am(III) was adsorbed also onto the resin from concentrated HNO3, and desorbed with 0.1 M HCl while keeping the Pu adsorbed. The on-column reduction of Pu(IV) to Pu(III) with 0.02 M TiCl3 facilitated the complete desorption of Pu. Interferences (e.g. Ca(2+), Fe(3+)) were washed off from the resin bed with excess HNO3. Using NdF3, micro-precipitates of the separated isotopes were prepared for analysis by both AMS and alpha spectrometry. The recovery was 97.7±5.3% and 95.5±4.6% for (241)Am and (242)Pu respectively in reagents without a matrix. The recoveries of the same isotopes were 99.1±6.0 and 96.8±5.3% respectively in garden soil. The robustness of the method was validated using certified reference materials (IAEA 384 and IAEA 385). The measurements agree with the certified values over a range of about 1-100 Bq kg(-1). The single column separation of Pu and Am saves reagents, separation time, and cost. PMID:24856406

  7. Isotope separation by photochromatography

    DOEpatents

    Suslick, Kenneth S.

    1977-01-01

    An isotope separation method which comprises physically adsorbing an isotopically mixed molecular species on an adsorptive surface and irradiating the adsorbed molecules with radiation of a predetermined wavelength which will selectively excite a desired isotopic species. Sufficient energy is transferred to the excited molecules to desorb them from the surface and thereby separate them from the unexcited undesired isotopic species. The method is particularly applicable to the separation of hydrogen isotopes.

  8. Isotope separation by photochromatography

    DOEpatents

    Suslick, K.S.

    1975-10-03

    A photochromatographic method for isotope separation is described. An isotopically mixed molecular species is adsorbed on an adsorptive surface, and the adsorbed molecules are irradiated with radiation of a predetermined wavelength which will selectively excite desired isotopic species. Sufficient energy is transferred to the excited molecules to desorb them from the surface and thus separate them from the undesired isotopic species. The method is particularly applicable to the separation of hydrogen isotopes. (BLM)

  9. Concordant plutonium-241-americium-241 dating of environmental samples: results from forest fire ash

    SciTech Connect

    Goldstein, Steven J; Oldham, Warren J; Murrell, Michael T; Katzman, Danny

    2010-12-07

    We have measured the Pu, {sup 237}Np, {sup 241}Am, and {sup 151}Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant {sup 241}Pu (t{sub 1/2} = 14.4 y)-{sup 241}Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use {sup 242}/{sup 239}Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the nonglobal fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, {sup 151}Sm (t{sub 1/2} = 90 y). We find that forest fire ash concentrates actinides and fission products with {approx}1E10 atoms {sup 239}Pu/g and {approx}1E8 atoms {sup 151}Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that {sup 151}Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the {sup 151}Sm/{sup 239}Pu atom ratio for global fallout is {approx}0.164, in agreement with an independent estimate of 0.165 based on {sup 137}Cs fission yields for atmospheric weapons tests at the NTS. {sup 241}Pu-{sup 241}Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950's-early 1960's, consistent with a peak in NTS

  10. Assessment of Neptunium, Americium, and Curium in the Savannah River Site Environment

    SciTech Connect

    Carlton, W.H.

    1997-12-17

    A series of documents has been published in which the impact of various radionuclides released to the environment by Savannah River Site (SRS) operations has been assessed. The quantity released, the disposition of the radionuclides in the environment, and the dose to offsite individuals has been presented for activation products, carbon cesium, iodine, plutonium, selected fission products, strontium, technetium, tritium, uranium, and the noble gases. An assessment of the impact of nonradioactive mercury also has been published.This document assesses the impact of radioactive transuranics released from SRS facilities since the first reactor became operational late in 1953. The isotopes reported here are 239Np, 241Am, and 244Cm.

  11. Determining the americium transmutation rate and fission rate by post-irradiation examination within the scope of the ECRIX-H experiment

    NASA Astrophysics Data System (ADS)

    Lamontagne, J.; Pontillon, Y.; Esbelin, E.; Béjaoui, S.; Pasquet, B.; Bourdot, P.; Bonnerot, J. M.

    2013-09-01

    The ECRIX-H experiment aims to assess the feasibility of transmuting americium micro-dispersed in an inert magnesia matrix under a locally moderated neutron flux in the Phénix reactor. A first set of examinations demonstrated that pellet behaviour was satisfactory with moderate swelling at the end of the irradiation. Additional post-irradiation examinations needed to be conducted to confirm the high transmutation rate so as to definitively conclude on the success of the ECRIX-H experiment. This article presents and discusses the results of these new examinations. They confirm the satisfactory behaviour of the MgO matrix not only during the basic irradiation but also during post-irradiation thermal transients. These examinations also provide additional information on the behaviour of fission products both in the americium-based particles and in the MgO matrix. These results particularly validate the transmutation rate predicted by the calculation codes using several different analytical techniques. The fission rate is also determined. Moderate pellet swelling under irradiation (6.7 vol.%), while only 23% of the produced He and 4% of the fission gases were released from the fuel. No interaction between the pellets and the cladding. Formation of bubbles due to the precipitation of fission gases and He mainly in bubbles located inside the americium-based particles. These bubbles are the main cause of macroscopic swelling in the pellets. Well-crystallised structure of the MgO matrix which shows no amorphisation after irradiation despite the presence of fission products. The absence of any reaction of MgO with the americium-based phase, Formation of a PuO2-type crystalline phase from AmO1.62 particles following the Am transmutation process. A shielded electron probe micro-analyser (EPMA) 'CAMECA' Camebax equipped to collect and exploit the measurements using the 'SAMx' system. A Philips XL30 scanning electron microscope (SEM). Field acquisitions were performed thanks to

  12. Comparative XRPD and XAS study of the impact of the synthesis process on the electronic and structural environments of uranium-americium mixed oxides

    NASA Astrophysics Data System (ADS)

    Prieur, D.; Lebreton, F.; Martin, P. M.; Caisso, M.; Butzbach, R.; Somers, J.; Delahaye, T.

    2015-10-01

    Uranium-americium mixed oxides are potential compounds to reduce americium inventory in nuclear waste via a partitioning and transmutation strategy. A thorough assessment of the oxygen-to-metal ratio is paramount in such materials as it determines the important underlying electronic structure and phase relations, affecting both thermal conductivity of the material and its interaction with the cladding and coolant. In 2011, various XAS experiments on U1-xAmxO2±δ samples prepared by different synthesis methods have reported contradictory results on the charge distribution of U and Am. This work alleviates this discrepancy. The XAS results confirm that, independently of the synthesis process, the reductive sintering of U1-xAmxO2±δ leads to the formation of similar fluorite solid solution indicating the presence of Am+III and U+V in equimolar proportions.

  13. Implications of Plutonium isotopic separation on closed fuel cycles and repository design

    SciTech Connect

    Forsberg, C.

    2013-07-01

    Advances in laser enrichment may enable relatively low-cost plutonium isotopic separation. This would have large impacts on LWR closed fuel cycles and waste management. If Pu-240 is removed before recycling plutonium as mixed oxide (MOX) fuel, it would dramatically reduce the buildup of higher plutonium isotopes, Americium, and Curium. Pu-240 is a fertile material and thus can be replaced by U-238. Eliminating the higher plutonium isotopes in MOX fuel increases the Doppler feedback, simplifies reactor control, and allows infinite recycle of MOX plutonium in LWRs. Eliminating fertile Pu-240 and Pu-242 reduces the plutonium content in MOX fuel and simplifies fabrication. Reducing production of Pu-241 reduces production of Am-241 - the primary heat generator in spent nuclear fuels after several decades. Reducing heat generating Am-241 would reduce repository cost and waste toxicity. Avoiding Am- 241 avoids its decay product Np-237, a nuclide that partly controls long-term oxidizing repository performance. Most of these benefits also apply to LWR plutonium recycled into fast reactors. There are benefits for plutonium isotopic separation in fast reactor fuel cycles (particularly removal of Pu-242) but the benefits are less. (author)

  14. Comparative XRPD and XAS study of the impact of the synthesis process on the electronic and structural environments of uranium–americium mixed oxides

    SciTech Connect

    Prieur, D.; Lebreton, F.; Somers, J.; Delahaye, T.

    2015-10-15

    Uranium–americium mixed oxides are potential compounds to reduce americium inventory in nuclear waste via a partitioning and transmutation strategy. A thorough assessment of the oxygen-to-metal ratio is paramount in such materials as it determines the important underlying electronic structure and phase relations, affecting both thermal conductivity of the material and its interaction with the cladding and coolant. In 2011, various XAS experiments on U{sub 1−x}Am{sub x}O{sub 2±δ} samples prepared by different synthesis methods have reported contradictory results on the charge distribution of U and Am. This work alleviates this discrepancy. The XAS results confirm that, independently of the synthesis process, the reductive sintering of U{sub 1−x}Am{sub x}O{sub 2±δ} leads to the formation of similar fluorite solid solution indicating the presence of Am{sup +III} and U{sup +V} in equimolar proportions. - Graphical abstract: Formation of (U{sup IV/V},Am{sup III})O{sup 2} solid solution by sol–gel and by powder metallurgy. - Highlights: • Uranium–americium mixed oxides were synthesized by sol–gel and powder metallurgy. • Fluorite solid solutions with similar local environment have been obtained. • U{sup V} and Am{sup III} are formed in equimolar proportions.

  15. METHOD OF ISOTOPE CONCENTRATION

    DOEpatents

    Spevack, J.S.

    1957-04-01

    An isotope concentration process is described which consists of exchanging, at two or more different temperature stages, two isotopes of an element between substances that are physically separate from each other and each of which is capable of containing either of the isotopes, and withdrawing from a point between at least two of the temperatare stages one of the substances containing an increased concentration of the desired isotope.

  16. Cosmic ray isotopes

    NASA Technical Reports Server (NTRS)

    Stone, E. C.

    1973-01-01

    The isotopic composition of cosmic rays is studied in order to develop the relationship between cosmic rays and stellar processes. Cross section and model calculations are reported on isotopes of H, He, Be, Al and Fe. Satellite instrument measuring techniques separate only the isotopes of the lighter elements.

  17. Statistical clumped isotope signatures

    PubMed Central

    Röckmann, T.; Popa, M. E.; Krol, M. C.; Hofmann, M. E. G.

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a molecule, which is the conventional reference. When multiple indistinguishable atoms of the same element are present in a molecule, this reference is calculated from the bulk (≈average) isotopic composition of the involved atoms. We show here that this referencing convention leads to apparent negative clumped isotope anomalies (anti-clumping) when the indistinguishable atoms originate from isotopically different populations. Such statistical clumped isotope anomalies must occur in any system where two or more indistinguishable atoms of the same element, but with different isotopic composition, combine in a molecule. The size of the anti-clumping signal is closely related to the difference of the initial isotope ratios of the indistinguishable atoms that have combined. Therefore, a measured statistical clumped isotope anomaly, relative to an expected (e.g. thermodynamical) clumped isotope composition, may allow assessment of the heterogeneity of the isotopic pools of atoms that are the substrate for formation of molecules. PMID:27535168

  18. Zirconium isotope separation

    SciTech Connect

    Siddall, M.B.

    1984-12-11

    A method of separating zirconium isotopes by converting the zirconium to its iodide salt prior to separation by usual isotope methods is disclosed. After separation the desired isotopes are converted from the salt to the metal by the van Arkel-de Boer iodide process.

  19. Statistical clumped isotope signatures.

    PubMed

    Röckmann, T; Popa, M E; Krol, M C; Hofmann, M E G

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a molecule, which is the conventional reference. When multiple indistinguishable atoms of the same element are present in a molecule, this reference is calculated from the bulk (≈average) isotopic composition of the involved atoms. We show here that this referencing convention leads to apparent negative clumped isotope anomalies (anti-clumping) when the indistinguishable atoms originate from isotopically different populations. Such statistical clumped isotope anomalies must occur in any system where two or more indistinguishable atoms of the same element, but with different isotopic composition, combine in a molecule. The size of the anti-clumping signal is closely related to the difference of the initial isotope ratios of the indistinguishable atoms that have combined. Therefore, a measured statistical clumped isotope anomaly, relative to an expected (e.g. thermodynamical) clumped isotope composition, may allow assessment of the heterogeneity of the isotopic pools of atoms that are the substrate for formation of molecules. PMID:27535168

  20. Management of Heavy Isotope in the DOE Complex

    SciTech Connect

    Canon, R.; Croff, A.; Boyd, L.

    2002-02-27

    cost to the user of obtaining newly produced material. The HIMG has also prepared issue papers on neptunium and americium/curium that identify the resources, potential uses, and disposal pathways for the materials across the DOE Complex. In the future the HIMG expects to comprehensively identify the status of the U.S. heavy isotope inventory, prepare additional issue papers and plans charting the future of this inventory, and to facilitate execution of the plan.

  1. Sorption of americium in tuff and pure minerals using synthetic and natural groundwaters

    SciTech Connect

    Triay, I.R.; Meijer, A.; Cisneros, M.R.; Miller, G.G.; Mitchell, A.J.; Ott, M.A.; Hobart, D.E.; Palmer, P.D.; Perrin, R.E.; Aguilar, R.D.

    1989-12-01

    The distribution of Am between selected solid and liquid phases has been studied using initial {sup 241}Am solutions with a molarity smaller than 1 {times} 10{sup {minus}11}. The synthetic and natural groundwaters used have pH values in the 7--8 range and a total alkalinity of approximately 1 mN which is mainly due to bicarbonate. Mass spectrometric isotope dilution was utilized to determine the amount of Am in the solution phase initially and after equilibrium was attained. Using this sensitive technique, 7 {times} 10{sup 8} atoms of {sup 241}Am were accurately measured. Our results indicate that the percent of Am lost to the walls of the container in the absence of geologic material varies from 35 to 84. The Am sorption coefficient determined is on the order of 10{sup 3} ml/g for clinoptilolite, 10{sup 4} ml/g for tuff consisting mainly of alkali feldspar and cristobalite, and 10{sup 5} ml/g for romanechite. 12 refs.

  2. Evaluation of synthetic water-soluble metal-binding polymers with ultrafiltration for selective concentration of americium and plutonium

    SciTech Connect

    Smith, B.F.; Gibson, R.R.; Jarvinen, G.D.; Jones, M.M.; Lu, M.T.; Robison, T.W.; Schroeder, N.C.; Stalnaker, N.

    1997-12-31

    Routine counting methods and ICP-MS are unable to directly measure the new US Department of Energy (DOE) regulatory level for discharge waters containing alpha-emitting radionuclides of 30 pCi/L total alpha or the 0.05 pCi/L regulatory level for Pu or Am activity required for surface waters at the Rocky Flats site by the State of Colorado. This inability indicates the need to develop rapid, reliable, and robust analytical techniques for measuring actinide metal ions, particularly americium and plutonium. Selective separation or preconcentration techniques would aid in this effort. Water-soluble metal-binding polymers in combination with ultrafiltration are shown to be an effective method for selectively removing dilute actinide ions from acidic solutions of high ionic strength. The actinide-binding properties of commercially available water-soluble polymers and several polymers which have been reported in the literature were evaluated. The functional groups incorporated in the polymers were pyrrolidone, amine, oxime, and carboxylic, phosphonic, or sulfonic acid. The polymer containing phosphonic acid groups gave the best results with high distribution coefficients and concentration factors for {sup 241}Am(III) and {sup 238}Pu(III)/(IV) at pH 4 to 6 and ionic strengths of 0.1 to 4.

  3. EURADOS INTERCOMPARISON ON MEASUREMENTS AND MONTE CARLO MODELLING FOR THE ASSESSMENT OF AMERICIUM IN A USTUR LEG PHANTOM

    SciTech Connect

    Lopez, M. A.; Broggio, D.; Capello, K.; Cardenas-Mendez, E.; El-Faramawy, N.; Franck, D.; James, Anthony C.; Kramer, Gary H.; Lacerenza, G.; Lynch, Timothy P.; Navarro, J. F.; Navarro, T.; Perez, B.; Ruhm, W.; Tolmachev, Sergei Y.; Weitzenegger, E.

    2011-03-01

    United States Transuranium and Uranium Registries (USTUR) Case 0102 was the first whole-body donation to the USTUR (1979), of a worker affected by a substantial accidental 241Am intake(1). Half of this man’s skeleton, encased in tissue-quivalent plastic, provides a unique human ‘phantom’ for calibrating in vivo counting systems. In this case, the 241Am skeletal activity was measured 25 y after the intake. Approximately 82 % of the 241Am remaining in the body was found in the bones and teeth. The241Am activity concentration throughout the skeleton (in all types of bone) was fairly uniform(2). A protocol has been proposed by a group of in vivo laboratories from Europe [CIEMAT-Spain, IRSN-France and Helmholtz Zentrum Mu¨nchen (HMGU)-Germany] and Canada (HML) participating in this DOS/USTUR intercomparison. The focus areas for the study included: (1) the efficiency pattern along the leg phantom using Germanium detectors (experimental and computational), (2) the comparison of Monte Carlo (MC) results with experimental values in counting efficiency data and (3) the inflence of americium distribution in the bone material (volume or surface).

  4. Chemical Speciation of Strontium, Americium, and Curium in High Level Waste: Predictive Modeling of Phase Partitioning During Tank Processing

    SciTech Connect

    Felmy, Andrew R.; Choppin, Gregory; Dixon, David A.; Campbell, James A.

    1999-06-01

    In this research program, Pacific Northwest National Laboratory (PNNL) and Florida State University (FSU) are investigating the speciation of strontium and americium/curium in the presence of selected organic chelating agents (ethylenediaminetetraacetic acid (EDTA), N-(2-hydroxyethyl) aethylenediaminetriacetic 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 project is composed of integrated research tasks that approach the problem of chemical speciation using macroscopic thermodynamic measurements of metal-ligand competition reactions, molecular modeling studies to identify structures or complexes of unusual stability, and mass spectrometry measurements of complex charge/mass ratio that can be applied to mixed metal-chelate systems. This fundamental information is then used to develop thermodynamic models, which allow the prediction of changes in chemical speciation and solubility that can occur in response to changes in tank processing conditions. In this way, we can develop new approaches that address fundamental problems in aqueous speciation and at the same time provide useful and practical information needed for tank processing.

  5. Intramolecular sensitization of americium luminescence in solution: Shining light on short-lived forbidden 5f transitions

    SciTech Connect

    Sturzbecher-Hoehne, M.; Yang, P.; D'Aleo, A.; Abergel, R. J.

    2016-01-01

    In this study, the photophysical properties and solution thermodynamics of water soluble trivalent americium (AmIII) complexes formed with multidentate chromophore-bearing ligands, 3,4,3-LI(1,2-HOPO), Enterobactin, and 5-LIO(Me-3,2-HOPO), were investigated. The three chelators were shown to act as antenna chromophores for AmIII, generating sensitized luminescence emission from the metal upon complexation, with very short lifetimes ranging from 33 to 42 ns and low luminescence quantum yields (10–3 to 10–2%), characteristic of Near Infra-Red emitters in similar systems. The specific emission peak of AmIII assigned to the 5D17F1 f–f transition was exploited to characterize the high proton-independent stability of the complex formed with the most efficient sensitizer 3,4,3-LI(1,2-HOPO), with a log β110 = 20.4 ± 0.2 value. In addition, the optical and solution thermodynamic features of these AmIII complexes, combined with density functional theory calculations, were used to probe the influence of electronic structure on coordination properties across the f-element series and to gain insight into ligand field effects.

  6. Intramolecular sensitization of americium luminescence in solution: Shining light on short-lived forbidden 5f transitions

    DOE PAGESBeta

    Sturzbecher-Hoehne, M.; Yang, P.; D'Aleo, A.; Abergel, R. J.

    2016-01-01

    In this study, the photophysical properties and solution thermodynamics of water soluble trivalent americium (AmIII) complexes formed with multidentate chromophore-bearing ligands, 3,4,3-LI(1,2-HOPO), Enterobactin, and 5-LIO(Me-3,2-HOPO), were investigated. The three chelators were shown to act as antenna chromophores for AmIII, generating sensitized luminescence emission from the metal upon complexation, with very short lifetimes ranging from 33 to 42 ns and low luminescence quantum yields (10–3 to 10–2%), characteristic of Near Infra-Red emitters in similar systems. The specific emission peak of AmIII assigned to the 5D1 → 7F1 f–f transition was exploited to characterize the high proton-independent stability of the complex formedmore » with the most efficient sensitizer 3,4,3-LI(1,2-HOPO), with a log β110 = 20.4 ± 0.2 value. In addition, the optical and solution thermodynamic features of these AmIII complexes, combined with density functional theory calculations, were used to probe the influence of electronic structure on coordination properties across the f-element series and to gain insight into ligand field effects.« less

  7. Theoretical investigation of pressure-induced structural transitions in americium using GGA+U and hybrid density functional theory methods

    NASA Astrophysics Data System (ADS)

    Verma, Ashok K.; Modak, P.; Sharma, Surinder M.; Svane, A.; Christensen, N. E.; Sikka, S. K.

    2013-07-01

    First-principles calculations have been performed for americium (Am) metal using the generalized gradient approximation + orbital-dependent onsite Coulomb repulsion via Hubbard interaction (GGA+U) and hybrid density functional theory (HYB-DFT) methods to investigate various ground state properties and pressure-induced structural transitions. Both methods yield equilibrium volume and bulk modulus in good agreement with the experimental results. The GGA+spin orbit coupling+U method reproduced all structural transitions under pressure correctly, but the HYB-DFT method failed to reproduce the observed Am-I to Am-II transition. Good agreement was found between calculated and experimental equations of states for all phases, but the first three phases need larger U (α) parameters (where α represents the fraction of Hartree-Fock exchange energy replacing the DFT exchange energy) than the fourth phase in order to match the experimental data. Thus, neither the GGA+U nor the HYB-DFT methods are able to describe the energetics of Am metal properly in the entire pressure range from 0 GPa to 50 GPa with a single choice of their respective U and α parameters. Low binding-energy peaks in the experimental photoemission spectrum at ambient pressure relate, for some parameter choices, well to peak positions in the calculated density of states function of Am-I.

  8. Nano-cerium vanadate: a novel inorganic ion exchanger for removal of americium and uranium from simulated aqueous nuclear waste.

    PubMed

    Banerjee, Chayan; Dudwadkar, Nilesh; Tripathi, Subhash Chandra; Gandhi, Pritam Maniklal; Grover, Vinita; Kaushik, Chetan Prakash; Tyagi, Avesh Kumar

    2014-09-15

    Cerium vanadate nanopowders were synthesized by a facile low temperature co-precipitation method. The product was characterized by X-ray diffraction and transmission electron microscopy and found to consist of ∼25 nm spherical nanoparticles. The efficiency of these nanopowders for uptake of alpha-emitting radionuclides (233)U (4.82 MeV α) and (241)Am (5.49 MeV α, 60 keV γ) has been investigated. Thermodynamically and kinetically favorable uptake of these radionuclides resulted in their complete removal within 3h from aqueous acidic feed solutions. The uptake capacity was observed to increase with increase in pH as the zeta potential value decreased with the increase in pH but effect of ionic strength was insignificant. Little influence of the ions like Sr(2+), Ru(3+), Fe(3+), etc., in the uptake process indicated CeVO4 nanopowders to be amenable for practical applications. The isotherms indicated predominant uptake of the radioactive metal ions in the solid phase of the exchanger at lower feed concentrations and linear Kielland plots with positive slopes indicated favorable exchange of the metal ions with the nanopowder. Performance comparison with the other sorbents reported indicated excellent potential of nano-cerium vanadate for removing americium and uranium from large volumes of aqueous acidic solutions. PMID:25128895

  9. Intramolecular sensitization of americium luminescence in solution: shining light on short-lived forbidden 5f transitions.

    PubMed

    Sturzbecher-Hoehne, M; Yang, P; D'Aléo, A; Abergel, R J

    2016-06-14

    The photophysical properties and solution thermodynamics of water soluble trivalent americium (Am(III)) complexes formed with multidentate chromophore-bearing ligands, 3,4,3-LI(1,2-HOPO), Enterobactin, and 5-LIO(Me-3,2-HOPO), were investigated. The three chelators were shown to act as antenna chromophores for Am(III), generating sensitized luminescence emission from the metal upon complexation, with very short lifetimes ranging from 33 to 42 ns and low luminescence quantum yields (10(-3) to 10(-2)%), characteristic of Near Infra-Red emitters in similar systems. The specific emission peak of Am(III) assigned to the (5)D1 → (7)F1 f-f transition was exploited to characterize the high proton-independent stability of the complex formed with the most efficient sensitizer 3,4,3-LI(1,2-HOPO), with a log β110 = 20.4 ± 0.2 value. In addition, the optical and solution thermodynamic features of these Am(III) complexes, combined with density functional theory calculations, were used to probe the influence of electronic structure on coordination properties across the f-element series and to gain insight into ligand field effects. PMID:26961598

  10. ISOTOPE CONVERSION DEVICE

    DOEpatents

    Wigner, E.P.; Young, G.J.; Ohlinger, L.A.

    1957-12-01

    This patent relates to nuclear reactors of tbe type utilizing a liquid fuel and designed to convert a non-thermally fissionable isotope to a thermally fissionable isotope by neutron absorption. A tank containing a reactive composition of a thermally fissionable isotope dispersed in a liquid moderator is disposed within an outer tank containing a slurry of a non-thermally fissionable isotope convertible to a thermally fissionable isotope by neutron absorption. A control rod is used to control the chain reaction in the reactive composition and means are provided for circulating and cooling the reactive composition and slurry in separate circuits.

  11. Isotopically controlled semiconductors

    SciTech Connect

    Haller, Eugene E.

    2001-12-21

    Semiconductor bulk crystals and multilayer structures with controlled isotopic composition have attracted much scientific and technical interest in the past few years. Isotopic composition affects a large number of physical properties, including phonon energies and lifetimes, bandgaps, the thermal conductivity and expansion coefficient and spin-related effects. Isotope superlattices are ideal media for self-diffusion studies. In combination with neutron transmutation doping, isotope control offers a novel approach to metal-insulator transition studies. Spintronics, quantum computing and nanoparticle science are emerging fields using isotope control.

  12. RFNC-VNIIEF Capabilities to Production High Pure Isotopes for Scientific and Medical Applications

    SciTech Connect

    Vesnovskii, S. P.

    2002-02-26

    In the technical paper there is presented the information on the basic equipment and more than thirty-year experience of RFNC-VNIIEF activities in the sphere of producing highly enriched isotopes of actinide elements--thorium, uranium, neptunium, plutonium, americium and curium--for scientific researches and practical applications. Electromagnetic separator and radiochemical methods provide obtaining of superpure isotope samples for nuclear-physical radiometric and mass-spectrometric equipment, and also as tracers when analyzing environmental contamination. There are presented the structure of the laboratory occupied with these isotopes electromagnetic separation as well as the nomenclature and characteristics of the specimens supplied. There are stated science and engineering elaborations of technologies aimed at producing alpha-ray radiating radionuclides--thorium-229, thorium-228, actinium-225, radium-224--for the purpose of anti-cancer therapy using bismuth-212 and bismuth-213 produced by the specially developed generators. There are presented the basic directions of cooperation with other Russian Institutes in developing this promising line of conversion.

  13. Direct isotope ratio analysis of individual uranium-plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry.

    PubMed

    Suzuki, Daisuke; Esaka, Fumitaka; Miyamoto, Yutaka; Magara, Masaaki

    2015-02-01

    Uranium and plutonium isotope ratios in individual uranium-plutonium (U-Pu) mixed particles with various U/Pu atomic ratios were analyzed without prior chemical separation by thermal ionization mass spectrometry (TIMS). Prior to measurement, micron-sized particles with U/Pu ratios of 1, 5, 10, 18, and 70 were produced from uranium and plutonium certified reference materials. In the TIMS analysis, the peaks of americium, plutonium, and uranium ion signals were successfully separated by continuously increasing the evaporation filament current. Consequently, the uranium and plutonium isotope ratios, except the (238)Pu/(239)Pu ratio, were successfully determined for the particles at all U/Pu ratios. This indicates that TIMS direct analysis allows for the measurement of individual U-Pu mixed particles without prior chemical separation. PMID:25479434

  14. Hybrid isotope separation scheme

    DOEpatents

    Maya, Jakob

    1991-01-01

    A method of yielding selectively a desired enrichment in a specific isotope including the steps of inputting into a spinning chamber a gas from which a scavenger, radiating the gas with a wave length or frequency characteristic of the absorption of a particular isotope of the atomic or molecular gas, thereby inducing a photochemical reaction between the scavenger, and collecting the specific isotope-containing chemical by using a recombination surface or by a scooping apparatus.

  15. HYDROGEN ISOTOPE TARGETS

    DOEpatents

    Ashley, R.W.

    1958-08-12

    The design of targets for use in the investigation of nuclear reactions of hydrogen isotopes by bombardment with accelerated particles is described. The target con struction eomprises a backing disc of a metal selected from the group consisting of molybdenunn and tungsten, a eoating of condensed titaniunn on the dise, and a hydrogen isotope selected from the group consisting of deuterium and tritium absorbed in the coatiag. The proeess for preparing these hydrogen isotope targets is described.

  16. Hybrid isotope separation scheme

    DOEpatents

    Maya, J.

    1991-06-18

    A method is described for yielding selectively a desired enrichment in a specific isotope including the steps of inputting into a spinning chamber a gas from which a scavenger, radiating the gas with a wave length or frequency characteristic of the absorption of a particular isotope of the atomic or molecular gas, thereby inducing a photochemical reaction between the scavenger, and collecting the specific isotope-containing chemical by using a recombination surface or by a scooping apparatus. 2 figures.

  17. Decorporation of systemically distributed americium by a novel orally administered diethylenetriaminepentaacetic acid (DTPA) formulation in beagle dogs.

    PubMed

    Wilson, James P; Cobb, Ronald R; Dungan, Nathanael W; Matthews, Laura L; Eppler, Bärbel; Aiello, Kenneth V; Curtis, Shiro; Boger, Teannetta; Guilmette, Raymond A; Weber, Waylon; Doyle-Eisele, Melanie; Talton, James D

    2015-03-01

    Novel decorporation agents are being developed to protect against radiological accidents and terrorists attacks. Radioactive americium is a significant component of nuclear fallout. Removal of large radioactive materials, such as 241Am, from exposed persons is a subject of significant interest due to the hazards they pose. The objective of this study was to evaluate the dose-related efficacy of daily doses of NanoDTPA™ Capsules for decorporating Am administered intravenously as a soluble citrate complex to male and female beagle dogs. In addition, the efficacy of the NanoDTPA™ Capsules for decorporating 241Am was directly compared to intravenously administered saline and DTPA. Animals received a single IV administration of 241Am(III)-citrate on Day 0. One day after radionuclide administration, one of four different doses of NanoDTPA™ Capsules [1, 2, or 6 capsules d(-1) (30 mg, 60 mg, or 180 mg DTPA) or 2 capsules BID], IV Zn-DTPA (5 mg kg(-1) pentetate zinc trisodium) as a positive control, or IV saline as a placebo were administered. NanoDTPA™ Capsules, IV Zn-DTPA, or IV saline was administered on study days 1-14. Animals were euthanized on day 21. A full necropsy was conducted, and liver, spleen, kidneys, lungs and trachea, tracheobronchial lymph nodes (TBLN), muscle samples (right and left quadriceps), gastrointestinal (GI) tract (stomach plus esophagus, upper and lower intestine), gonads, two femurs, lumbar vertebrae (L1-L4), and all other soft tissue remains were collected. Urinary and fecal excretion profiles were increased approximately 10-fold compared to those for untreated animals. Tissue contents were decreased compared to untreated controls. In particular, liver content was decreased by approximately eightfold compared to untreated animals. The results from this study further demonstrate that oral NanoDTPA™ Capsules are equally efficient compared to IV Zn-DTPA in decorporation of actinides. PMID:25627942

  18. The DOE Isotopes Program

    NASA Astrophysics Data System (ADS)

    Gillo, Jehannes

    2015-10-01

    The DOE Isotope Program is a small federal program with a great deal of impact and is managed by the DOE Office of Nuclear Physics. The Isotope Program has been managed by the Office of Nuclear Physics since 2009, and since that time, has been re-defined in terms of mission, scope and operations. The program produces critical isotopes that are in short supply or simply unavailable from elsewhere to facilitate research and applications. Research is also supported to develop or improve production techniques that will increase availability of isotopes in high demand, such as alpha emitters for cancer therapy.

  19. Measurement of total alpha activity of neptunium, plutonium, and americium in highly radioactive Hanford waste by iron hydroxide precipitation and 2-heptanone solvent extraction

    SciTech Connect

    Maiti, T.C.; Kaye, J.H.

    1992-06-01

    An improved method has been developed to concentrate the major alpha-emitting actinide elements neptunium, plutonium, and americium from samples with high salt content such as those resulting from efforts to characterize Hanford storage tank waste. Actinide elements are concentrated by coprecipitation of their hydroxides using iron carrier. The iron is removed by extraction from 8M HCI with 2-heptanone. The actinide elements remain in the aqueous phase free from salts, iron, and long-lived fission products. Recoveries averaged 98 percent.

  20. Isotopically engineered semiconductors

    NASA Astrophysics Data System (ADS)

    Haller, E. E.

    1995-04-01

    Scientific interest, technological promise, and increased availability of highly enriched isotopes have led to a sharp rise in the number of experimental and theoretical studies with isotopically controlled semiconductor crystals. This review of mostly recent activities begins with an introduction to some past classical experiments which have been performed on isotopically controlled semiconductors. A review of the natural isotopic composition of the relevant elements follows. Some materials aspects resulting in part from the high costs of enriched isotopes are discussed next. Raman spectroscopy studies with a number of isotopically pure and deliberately mixed Ge bulk crystals show that the Brillouin-zone-center optical phonons are not localized. Their lifetime is almost independent of isotopic disorder, leading to homogeneous Raman line broadening. Studies with short period isotope superlattices consisting of alternating layers of n atomic planes of 70Ge and 74Ge reveal a host of zone-center phonons due to Brillouin-zone folding. At n≳40 one observes two phonon lines at frequencies corresponding to the bulk values of the two isotopes. In natural diamond, isotope scattering of the low-energy phonons, which are responsible for the thermal conductivity, is very strongly affected by small isotope disorder. Isotopically pure 12C diamond crystals exhibit thermal conductivities as high as 410 W cm-1 K-1 at 104 K, leading to projected values of over 2000 W cm-1 K-1 near 80 K. The changes in phonon properties with isotopic composition also weakly affect the electronic band structures and the lattice constants. The latter isotope dependence is most relevant for future standards of length based on crystal lattice constants. Capture of thermal neutrons by isotope nuclei followed by nuclear decay produces new elements, resulting in a very large number of possibilities for isotope selective doping of semiconductors. This neutron transmutation of isotope nuclei, already used

  1. Fabrication and characterization of U1-xAmxO2±δ compounds with high americium contents (x = 0.3, 0.4 and 0.5)

    NASA Astrophysics Data System (ADS)

    Lebreton, Florent; Horlait, Denis; Delahaye, Thibaud; Blanchart, Philippe

    2013-08-01

    Mixed uranium-americium oxides are considered promising compounds for americium transmutation in fast neutron reactors. A better understanding of these materials and of the U-Am-O phase diagram is, however, needed. Though many results in the literature describe U1-xAmxO2±δ (x ⩽ 0.2) compounds, very few studies concern higher Am contents. In this context, this article reports the fabrication method of U1-xAmxO2±δ (0.3 ⩽ x ⩽ 0.5) and their preliminary characterization, notably by X-ray diffraction.

  2. Intracellular Cadmium Isotope Fractionation

    NASA Astrophysics Data System (ADS)

    Horner, T. J.; Lee, R. B.; Henderson, G. M.; Rickaby, R. E.

    2011-12-01

    Recent stable isotope studies into the biological utilization of transition metals (e.g. Cu, Fe, Zn, Cd) suggest several stepwise cellular processes can fractionate isotopes in both culture and nature. However, the determination of fractionation factors is often unsatisfactory, as significant variability can exist - even between different organisms with the same cellular functions. Thus, it has not been possible to adequately understand the source and mechanisms of metal isotopic fractionation. In order to address this problem, we investigated the biological fractionation of Cd isotopes within genetically-modified bacteria (E. coli). There is currently only one known biological use or requirement of Cd, a Cd/Zn carbonic anhydrase (CdCA, from the marine diatom T. weissfloggii), which we introduce into the E. coli genome. We have also developed a cleaning procedure that allows for the treating of bacteria so as to study the isotopic composition of different cellular components. We find that whole cells always exhibit a preference for uptake of the lighter isotopes of Cd. Notably, whole cells appear to have a similar Cd isotopic composition regardless of the expression of CdCA within the E. coli. However, isotopic fractionation can occur within the genetically modified E. coli during Cd use, such that Cd bound in CdCA can display a distinct isotopic composition compared to the cell as a whole. Thus, the externally observed fractionation is independent of the internal uses of Cd, with the largest Cd isotope fractionation occurring during cross-membrane transport. A general implication of these experiments is that trace metal isotopic fractionation most likely reflects metal transport into biological cells (either actively or passively), rather than relating to expression of specific physiological function and genetic expression of different metalloenzymes.

  3. Discovery of the krypton isotopes

    SciTech Connect

    Heim, M.; Fritsch, A.; Schuh, A.; Shore, A.; Thoennessen, M.

    2010-07-15

    Thirty-two krypton isotopes have been observed so far and the discovery of these isotopes is discussed here. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  4. (Carbon isotope fractionation inplants)

    SciTech Connect

    O'Leary, M.H.

    1990-01-01

    The objectives of this research are: To develop a theoretical and experimental framework for understanding isotope fractionations in plants; and to develop methods for using this isotope fractionation for understanding the dynamics of CO{sub 2} fixation in plants. Progress is described.

  5. Detecting isotopic ratio outliers

    SciTech Connect

    Bayne, C.K.; Smith, D.H.

    1985-01-01

    An alternative method is proposed for improving isotopic ratio estimates. This method mathematically models pulse-count data and uses iterative reweighted Poisson regression to estimate model parameters to calculate the isotopic ratios. This computer-oriented approach provides theoretically better methods than conventional techniques to establish error limits and to identify outliers. 6 refs., 3 figs., 3 tabs.

  6. Laser isotope separation

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Boyer, Keith; Greiner, Norman R.

    1988-01-01

    A process and apparatus for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photolysis, photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photolysis, photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium.

  7. Photochemical isotope separation

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

    1987-01-01

    A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

  8. Discovery of Isotopes

    NASA Astrophysics Data System (ADS)

    May, Erin; Thoennessen, Michael

    2011-10-01

    To date, no comprehensive study has been undertaken regarding the initial detection and identification of isotopes. At NSCL, a project has been initiated to catalog and report the initial observation of every isotope. The conditions characterizing the successful discovery of an isotope include a clear and unambiguous mass and element identification through decay curves, mass spectroscopy, gamma-ray spectra, and/or relationships to other isotopes, as well as the publication of such findings in a refereed journal. I will present the documentation for eight elements: cesium, lanthanum, praseodymium, promethium, samarium, europium, gadolinium, and terbium. The year and author of each initial publication along with the location and methods of production and identification will be shown. A summary and overview of all ~3000 isotopes documented so far as a function of discovery year, method and place will also be presented.

  9. Photochemical isotope separation

    DOEpatents

    Robinson, C.P.; Jensen, R.J.; Cotter, T.P.; Greiner, N.R.; Boyer, K.

    1987-04-28

    A process is described for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium. 8 figs.

  10. Laser isotope separation

    DOEpatents

    Robinson, C.P.; Reed, J.J.; Cotter, T.P.; Boyer, K.; Greiner, N.R.

    1975-11-26

    A process and apparatus for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light is described. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photolysis, photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photolysis, photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium.

  11. Synthesis of zirconia sol stabilized by trivalent cations (yttrium and neodymium or americium): a precursor for Am-bearing cubic stabilized zirconia.

    PubMed

    Lemonnier, Stephane; Grandjean, Stephane; Robisson, Anne-Charlotte; Jolivet, Jean-Pierre

    2010-03-01

    Recent concepts for nuclear fuel and targets for transmuting long-lived radionuclides (minor actinides) and for the development of innovative Gen-IV nuclear fuel cycles imply fabricating host phases for actinide or mixed actinide compounds. Cubic stabilized zirconia (Zr, Y, Am)O(2-x) is one of the mixed phases tested in transmutation experiments. Wet chemical routes as an alternative to the powder metallurgy are being investigated to obtain the required phases while minimizing the handling of contaminating radioactive powder. Hydrolysis of zirconium, neodymium (a typical surrogate for americium) and yttrium in aqueous media in the presence of acetylacetone was firstly investigated. Progressive hydrolysis of zirconium acetylacetonate and sorption of trivalent cations and acacH on the zirconia particles led to a stable dispersion of nanoparticles (5-7 nm) in the 6-7 pH range. This sol gels with time or with temperature. The application to americium-containing solutions was then successfully tested: a stable sol was synthesized, characterized and used to prepare cubic stabilized zirconia (Zr, Y, Am)O(2-x). PMID:20162199

  12. Isotopically controlled semiconductors

    SciTech Connect

    Haller, Eugene E.

    2006-06-19

    The following article is an edited transcript based on the Turnbull Lecture given by Eugene E. Haller at the 2005 Materials Research Society Fall Meeting in Boston on November 29, 2005. The David Turnbull Lectureship is awarded to recognize the career of a scientist who has made outstanding contributions to understanding materials phenomena and properties through research, writing, and lecturing, as exemplified by the life work of David Turnbull. Haller was named the 2005 David Turnbull Lecturer for his 'pioneering achievements and leadership in establishing the field of isotopically engineered semiconductors; for outstanding contributions to materials growth, doping and diffusion; and for excellence in lecturing, writing, and fostering international collaborations'. The scientific interest, increased availability, and technological promise of highly enriched isotopes have led to a sharp rise in the number of experimental and theoretical studies with isotopically controlled semiconductor crystals. This article reviews results obtained with isotopically controlled semiconductor bulk and thin-film heterostructures. Isotopic composition affects several properties such as phonon energies, band structure, and lattice constant in subtle, but, for their physical understanding, significant ways. Large isotope-related effects are observed for thermal conductivity in local vibrational modes of impurities and after neutron transmutation doping. Spectacularly sharp photoluminescence lines have been observed in ultrapure, isotopically enriched silicon crystals. Isotope multilayer structures are especially well suited for simultaneous self- and dopant-diffusion studies. The absence of any chemical, mechanical, or electrical driving forces makes possible the study of an ideal random-walk problem. Isotopically controlled semiconductors may find applications in quantum computing, nanoscience, and spintronics.

  13. ISOTOPE SEPARATING APPARATUS

    DOEpatents

    Kudravetz, M.K.; Greene, H.B.

    1958-09-16

    This patent relates to control systems for a calutron and, in particular, describes an electro-mechanical system for interrupting the collection of charged particles when the ratio between the two isotopes being receivcd deviates from a predetermined value. One embodiment of the invention includes means responsive to the ratio between two isotopes being received for opening a normally closed shutter over the receiver entrance when the isotope ratio is the desired value. In another form of the invention the collection operation is interrupted by changing the beam accelerating voltage to deflect the ion beam away from the receiver.

  14. Carbon isotope techniques

    SciTech Connect

    Coleman, D.C. ); Fry, B. )

    1991-01-01

    This book is a hands-on introduction to using carbon isotope tracers in experimental biology and ecology. It is a bench-top reference with protocols for the study of plants, animals, and soils. The {sup 11}C, {sup 12}C, {sup 13}C, and {sup 14}C carbon isotopes are considered and standard techniques are described by established authors. The compilation includes the following features: specific, well-established, user-oriented techniques; carbon cycles in plants, animals, soils, air, and water; isotopes in ecological research; examples and sample calculations.

  15. Stable isotopes in mineralogy

    USGS Publications Warehouse

    O'Neil, J.R.

    1977-01-01

    Stable isotope fractionations between minerals are functions of the fundamental vibrational frequencies of the minerals and therefore bear on several topics of mineralogical interest. Isotopic compositions of the elements H, C, O, Si, and S can now be determined routinely in almost any mineral. A summary has been made of both published and new results of laboratory investigations, analyses of natural materials, and theoretical considerations which bear on the importance of temperature, pressure, chemical composition and crystal structure to the isotopic properties of minerals. It is shown that stable isotope studies can sometimes provide evidence for elucidating details of crystal structure and can be a powerful tool for use in tracing the reaction paths of mineralogical reactions. ?? 1977 Springer-Verlag.

  16. Perchlorate isotope forensics

    USGS Publications Warehouse

    Böhlke, J.K.; Sturchio, N.C.; Gu, B.; Horita, J.; Brown, G.M.; Jackson, W.A.; Batista, J.; Hatzinger, P.B.

    2005-01-01

    Perchlorate has been detected recently in a variety of soils, waters, plants, and food products at levels that may be detrimental to human health. These discoveries have generated considerable interest in perchlorate source identification. In this study, comprehensive stable isotope analyses ( 37Cl/35Cl and 18O/17O/ 16O) of perchlorate from known synthetic and natural sources reveal systematic differences in isotopic characteristics that are related to the formation mechanisms. In addition, isotopic analyses of perchlorate extracted from groundwater and surface water demonstrate the feasibility of identifying perchlorate sources in contaminated environments on the basis of this technique. Both natural and synthetic sources of perchlorate have been identified in water samples from some perchlorate occurrences in the United States by the isotopic method. ?? 2005 American Chemical Society.

  17. Rare Isotope Accelerators

    NASA Astrophysics Data System (ADS)

    Savard, Guy

    2002-04-01

    The next frontier for low-energy nuclear physics involves experimentation with accelerated beams of short-lived radioactive isotopes. A new facility, the Rare Isotope Accelerator (RIA), is proposed to produce large amount of these rare isotopes and post-accelerate them to energies relevant for studies in nuclear physics, astrophysics and the study of fundamental interactions at low energy. The basic science motivation for this facility will be introduced. The general facility layout, from the 400 kW heavy-ion superconducting linac used for production of the required isotopes to the novel production and extraction schemes and the highly efficient post-accelerator, will be presented. Special emphasis will be put on a number of technical breakthroughs and recent R&D results that enable this new facility.

  18. Isotopically controlled semiconductors

    SciTech Connect

    Haller, E.E.

    2004-11-15

    A review of recent research involving isotopically controlled semiconductors is presented. Studies with isotopically enriched semiconductor structures experienced a dramatic expansion at the end of the Cold War when significant quantities of enriched isotopes of elements forming semiconductors became available for worldwide collaborations. Isotopes of an element differ in nuclear mass, may have different nuclear spins and undergo different nuclear reactions. Among the latter, the capture of thermal neutrons which can lead to neutron transmutation doping, can be considered the most important one for semiconductors. Experimental and theoretical research exploiting the differences in all the properties has been conducted and will be illustrated with selected examples. Manuel Cardona, the longtime editor-in-chief of Solid State Communications has been and continues to be one of the major contributors to this field of solid state physics and it is a great pleasure to dedicate this review to him.

  19. Oxygen isotope cosmothermometer.

    NASA Technical Reports Server (NTRS)

    Onuma, N.; Clayton, R. N.; Mayeda, T. K.

    1972-01-01

    Variations in oxygen isotopic abundances of meteoritic minerals, chondrules, whole meteorites, and planets are discussed in terms of a model involving isotopic exchange between primordial dust and a cooling solar nebular gas. From the temperature-dependence of the isotopic fractionation factors, temperatures have been assigned to the processes of initial condensation, chondrule formation, and planetary accretion. Separated phases from carbonaceous chondrites fall into three isotopic groups representing widely differing conditions of formation: (1) low-iron olivine and pyroxene, and calcium-aluminum silicates condensed at temperatures above 1000 K; (2) high-iron olivine and pyroxene melted to form chondrules after prior cooling and exchange to temperatures of 530-620 K; and (3) hydrous silicates condensed at temperatures below 400 K.

  20. Oxygen Isotopes in Meteorites

    NASA Astrophysics Data System (ADS)

    Clayton, R. N.

    2003-12-01

    Oxygen isotope abundance variations in meteorites are very useful in elucidating chemical and physical processes that occurred during the formation of the solar system (Clayton, 1993). On Earth, the mean abundances of the three stable isotopes are 16O: 99.76%, 17O: 0.039%, and 18O: 0.202%. It is conventional to express variations in abundances of the isotopes in terms of isotopic ratios, relative to an arbitrary standard, called SMOW (for standard mean ocean water), as follows:The isotopic composition of any sample can then be represented by one point on a "three-isotope plot," a graph of δ17O versus δ18O. It will be seen that such plots are invaluable in interpreting meteoritic data. Figure 1 shows schematically the effect of various processes on an initial composition at the center of the diagram. Almost all terrestrial materials lie along a "fractionation" trend; most meteoritic materials lie near a line of "16O addition" (or subtraction). (4K)Figure 1. Schematic representation of various isotopic processes shown on an oxygen three-isotope plot. Almost all terrestrial materials plot along a line of "fractionation"; most primitive meteoritic materials plot near a line of "16O addition." The three isotopes of oxygen are produced by nucleosynthesis in stars, but by different nuclear processes in different stellar environments. The principal isotope, 16O, is a primary isotope (capable of being produced from hydrogen and helium alone), formed in massive stars (>10 solar masses), and ejected by supernova explosions. The two rare isotopes are secondary nuclei (produced in stars from nuclei formed in an earlier generation of stars), with 17O coming primarily from low- and intermediate-mass stars (<8 solar masses), and 18O coming primarily from high-mass stars (Prantzos et al., 1996). These differences in type of stellar source result in large observable variations in stellar isotopic abundances as functions of age, size, metallicity, and galactic location ( Prantzos

  1. The structures of CyMe4-BTBP complexes of americium(iii) and europium(iii) in solvents used in solvent extraction, explaining their separation properties.

    PubMed

    Ekberg, Christian; Löfström-Engdahl, Elin; Aneheim, Emma; Foreman, Mark R StJ; Geist, Andreas; Lundberg, Daniel; Denecke, Melissa; Persson, Ingmar

    2015-11-14

    Separation of trivalent actinoid (An(iii)) and lanthanoid (Ln(iii)) ions is extremely challenging due to their similar ionic radii and chemical properties. Poly-aromatic nitrogen compounds acting as tetradentate chelating ligands to the metal ions in the extraction, have the ability to sufficiently separate An(iii) from Ln(iii). One of these compounds, 6,6'-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydro-benzol[1,2,4]triazin-3-yl)[2,2]bipyridine, CyMe4-BTBP, has proven to be resistant towards acidic environments and strong radiation from radioactive decomposition. EXAFS studies of the dicomplexes of CyMe4-BTBP with americium(iii) and europium(iii) in nitrobenzene, cyclohexanone, 1-hexanol, 1-octanol and malonamide (DMDOHEMA) in 1-octanol have been carried out to get a deeper understanding of the parameters responsible for the separation. The predominating complexes independent of solvent used are [Am(CyMe4-BTBP)2(NO3)](2+) and [Eu(CyMe4-BTBP)2](3+), respectively, which are present as outer-sphere ion-pairs with nitrate ions in the studied solvents with low relative permittivity. The presence of a nitrate ion in the first coordination sphere of the americium(iii) complex compensates the charge density of the complex considerably in comparison when only outer-sphere ion-pairs are formed as for the [Eu(CyMe4-BTBP)2](3+) complex. The stability and solubility of a complex in a solvent with low relative permittivity increase with decreasing charge density. The [Am(CyMe4-BTBP)2(NO3)](2+) complex will therefore be increasingly soluble and stabilized over the [Eu(CyMe4-BTBP)2](3+) complex in solvents with decreasing relative permittivity of the solvent. The separation of americium(iii) from europium(iii) with CyMe4-BTBP as extraction agent will increase with decreasing relative permittivity of the solvent, and thereby also with decreasing solubility of CyMe4-BTBP. The choice of solvent is therefore a balance of a high separation factor and sufficient solubility of the CyMe4-BTBP

  2. The isotopic distribution conundrum.

    PubMed

    Valkenborg, Dirk; Mertens, Inge; Lemière, Filip; Witters, Erwin; Burzykowski, Tomasz

    2012-01-01

    Although access to high-resolution mass spectrometry (MS), especially in the field of biomolecular MS, is becoming readily available due to recent advances in MS technology, the accompanied information on isotopic distribution in high-resolution spectra is not used at its full potential, mainly because of lack of knowledge and/or awareness. In this review, we give an insight into the practical problems related to calculating the isotopic distribution for large biomolecules, and present an overview of methods for the calculation of the isotopic distribution. We discuss the key events that triggered the development of various algorithms and explain the rationale of how and why the various isotopic-distribution calculations were performed. The review is focused around the developmental stages as briefly outlined below, starting with the first observation of an isotopic distribution. The observations of Beynon in the field of organic MS that chlorine appeared in a mass spectrum as two variants with odds 3:1 lie at the basis of the first wave of algorithms for the calculation of the isotopic distribution, based on the atomic composition of a molecule. From here on, we explain why more complex biomolecules such as peptides exhibit a highly complex isotope pattern when assayed by MS, and we discuss how combinatorial difficulties complicate the calculation of the isotopic distribution on computers. For this purpose, we highlight three methods, which were introduced in the 1980s. These are the stepwise procedure introduced by Kubinyi, the polynomial expansion from Brownawell and Fillippo, and the multinomial expansion from Yergey. The next development was instigated by Rockwood, who suggested to decompose the isotopic distribution in terms of their nucleon count instead of the exact mass. In this respect, we could claim that the term "aggregated" isotopic distribution is more appropriate. Due to the simplification of the isotopic distribution to its aggregated counterpart

  3. Physicochemical isotope anomalies

    SciTech Connect

    Esat, T.M.

    1988-06-01

    Isotopic composition of refractory elements can be modified, by physical processes such as distillation and sputtering, in unexpected patterns. Distillation enriches the heavy isotopes in the residue and the light isotopes in the vapor. However, current models appear to be inadequate to describe the detailed mass dependence, in particular for large fractionations. Coarse- and fine-grained inclusions from the Allende meteorite exhibit correlated isotope effects in Mg both as mass-dependent fractionation and residual anomalies. This isotope pattern can be duplicated by high temperature distillation in the laboratory. A ubiquitous property of meteoritic inclusions for Mg as well as for most of the other elements, where measurements exist, is mass-dependent fractionation. In contrast, terrestrial materials such as microtektites, tektite buttons as well as lunar orange and green glass spheres have normal Mg isotopic composition. A subset of interplanetary dust particles labelled as chondritic aggregates exhibit excesses in {sup 26}Mg and deuterium anomalies. Sputtering is expected to be a dominant mechanism in the destruction of grains within interstellar dust clouds. An active proto-sun as well as the present solar-wind and solar-flare flux are of sufficient intensity to sputter significant amounts of material. Laboratory experiments in Mg show widespread isotope effects including residual {sup 26}Mg excesses and mass dependent fractionation. It is possible that the {sup 26}Mg excesses in interplanetary dust is related to sputtering by energetic solar-wind particles. The implication if the laboratory distillation and sputtering effects are discussed and contrasted with the anomalies in meteoritic inclusions the other extraterrestrial materials the authors have access to.

  4. Isotopic geochemistry and cosmochemistry

    NASA Astrophysics Data System (ADS)

    Shchukoliukov, Iu. A.

    The book includes recent information on isotope geology, geochemistry, and cosmochemistry, discussed at a recent Soviet-Japanese symposium (at Irkutsk, USSR). Attention is given to numerical modeling of geochronometric systems, a classification of noble-gas components in the earth's interior, the feasibility of using ion microprobe for local isotope analysis of zircons for the purpose of deriving the early history of the earth (on the example of the Novopavlovsk complex from the Ukranian shield), a geological and geochronological study of the Ganalski complex of Kamchatka, and strontium isotopes as a criterion of the nature of acid melts (i.e., mantle- or crust-related). Other papers are on the geochronology and geology of Siberian kimberlites, the nature of sulfur from effusive rocks of the Kamchatka-Kuril-Japan island arc, mass-spectrometric studies of volatile components in exocontact rocks of alkaline-basic intrusions, and an analytical method for stable-isotope analysis in ultrasmall amounts of CO2 and its application to studies of the microscale isotopic zoning in calcite and graphite crystals in marble.

  5. Separation of sulfur isotopes

    DOEpatents

    DeWitt, Robert; Jepson, Bernhart E.; Schwind, Roger A.

    1976-06-22

    Sulfur isotopes are continuously separated and enriched using a closed loop reflux system wherein sulfur dioxide (SO.sub.2) is reacted with sodium hydroxide (NaOH) or the like to form sodium hydrogen sulfite (NaHSO.sub.3). Heavier sulfur isotopes are preferentially attracted to the NaHSO.sub.3, and subsequently reacted with sulfuric acid (H.sub.2 SO.sub.4) forming sodium hydrogen sulfate (NaHSO.sub.4) and SO.sub.2 gas which contains increased concentrations of the heavier sulfur isotopes. This heavy isotope enriched SO.sub.2 gas is subsequently separated and the NaHSO.sub.4 is reacted with NaOH to form sodium sulfate (Na.sub.2 SO.sub.4) which is subsequently decomposed in an electrodialysis unit to form the NaOH and H.sub.2 SO.sub.4 components which are used in the aforesaid reactions thereby effecting sulfur isotope separation and enrichment without objectionable loss of feed materials.

  6. Transportation of medical isotopes

    SciTech Connect

    Nielsen, D.L.

    1997-11-19

    A Draft Technical Information Document (HNF-1855) is being prepared to evaluate proposed interim tritium and medical isotope production at the Fast Flux Test Facility (FFTF). This assessment examines the potential health and safety impacts of transportation operations associated with the production of medical isotopes. Incident-free and accidental impacts are assessed using bounding source terms for the shipment of nonradiological target materials to the Hanford Site, the shipment of irradiated targets from the FFTF to the 325 Building, and the shipment of medical isotope products from the 325 Building to medical distributors. The health and safety consequences to workers and the public from the incident-free transportation of targets and isotope products would be within acceptable levels. For transportation accidents, risks to works and the public also would be within acceptable levels. This assessment is based on best information available at this time. As the medical isotope program matures, this analysis will be revised, if necessary, to support development of a final revision to the Technical Information Document.

  7. Isotope separation apparatus

    DOEpatents

    Arnush, Donald; MacKenzie, Kenneth R.; Wuerker, Ralph F.

    1980-01-01

    Isotope separation apparatus consisting of a plurality of cells disposed adjacent to each other in an evacuated container. A common magnetic field is established extending through all of the cells. A source of energetic electrons at one end of the container generates electrons which pass through the cells along the magnetic field lines. Each cell includes an array of collector plates arranged in parallel or in tandem within a common magnetic field. Sets of collector plates are disposed adjacent to each other in each cell. Means are provided for differentially energizing ions of a desired isotope by applying energy at the cyclotron resonant frequency of the desired isotope. As a result, the energized desired ions are preferentially collected by the collector plates.

  8. Atomic Weights and Isotopic Compositions

    National Institute of Standards and Technology Data Gateway

    SRD 144 Atomic Weights and Isotopic Compositions (Web, free access)   The atomic weights are available for elements 1 through 111, and isotopic compositions or abundances are given when appropriate.

  9. Nonbiological fractionation of iron isotopes

    NASA Technical Reports Server (NTRS)

    Anbar, A. D.; Roe, J. E.; Barling, J.; Nealson, K. H.

    2000-01-01

    Laboratory experiments demonstrate that iron isotopes can be chemically fractionated in the absence of biology. Isotopic variations comparable to those seen during microbially mediated reduction of ferrihydrite are observed. Fractionation may occur in aqueous solution during equilibration between inorganic iron complexes. These findings provide insight into the mechanisms of iron isotope fractionation and suggest that nonbiological processes may contribute to iron isotope variations observed in sediments.

  10. DEEP WATER ISOTOPIC CURRENT ANALYZER

    DOEpatents

    Johnston, W.H.

    1964-04-21

    A deepwater isotopic current analyzer, which employs radioactive isotopes for measurement of ocean currents at various levels beneath the sea, is described. The apparatus, which can determine the direction and velocity of liquid currents, comprises a shaft having a plurality of radiation detectors extending equidistant radially therefrom, means for releasing radioactive isotopes from the shaft, and means for determining the time required for the isotope to reach a particular detector. (AEC)

  11. Method for separating boron isotopes

    DOEpatents

    Rockwood, Stephen D.

    1978-01-01

    A method of separating boron isotopes .sup.10 B and .sup.11 B by laser-induced selective excitation and photodissociation of BCl.sub.3 molecules containing a particular boron isotope. The photodissociation products react with an appropriate chemical scavenger and the reaction products may readily be separated from undissociated BCl.sub.3, thus effecting the desired separation of the boron isotopes.

  12. Uranium Isotopic Analysis with the FRAM Isotopic Analysis Code

    SciTech Connect

    Duc T. Vo; Thomas E. Sampson

    1999-05-01

    FRAM is the acronym for Fixed-energy Response-function Analysis with Multiple efficiency. This software was developed at Los Alamos National Laboratory originally for plutonium isotopic analysis. Later, it was adapted for uranium isotopic analysis in addition to plutonium. It is a code based on a self-calibration using several gamma-ray peaks for determining the isotopic ratios. The versatile-parameter database structure governs all facets of the data analysis. User editing of the parameter sets allows great flexibility in handling data with different isotopic distributions, interfering isotopes, and different acquisition parameters such as energy calibration and detector type.

  13. Forensic Stable Isotope Biogeochemistry

    NASA Astrophysics Data System (ADS)

    Cerling, Thure E.; Barnette, Janet E.; Bowen, Gabriel J.; Chesson, Lesley A.; Ehleringer, James R.; Remien, Christopher H.; Shea, Patrick; Tipple, Brett J.; West, Jason B.

    2016-06-01

    Stable isotopes are being used for forensic science studies, with applications to both natural and manufactured products. In this review we discuss how scientific evidence can be used in the legal context and where the scientific progress of hypothesis revisions can be in tension with the legal expectations of widely used methods for measurements. Although this review is written in the context of US law, many of the considerations of scientific reproducibility and acceptance of relevant scientific data span other legal systems that might apply different legal principles and therefore reach different conclusions. Stable isotopes are used in legal situations for comparing samples for authenticity or evidentiary considerations, in understanding trade patterns of illegal materials, and in understanding the origins of unknown decedents. Isotope evidence is particularly useful when considered in the broad framework of physiochemical processes and in recognizing regional to global patterns found in many materials, including foods and food products, drugs, and humans. Stable isotopes considered in the larger spatial context add an important dimension to forensic science.

  14. Carbon Isotope Ratiometer

    SciTech Connect

    Dr. Anthony O'Keefe

    2001-05-07

    This Report details the design of a optical analyzer capable of measuring and recording the carbon 13/12 isotope ratio in atmospheric carbon dioxide. The system can operate in remote modes for long duration and will transmit real-time data via wireless contact.

  15. Sulfur isotopic data

    SciTech Connect

    Rye, R.O.

    1987-01-01

    Preliminary sulfur isotope data have been determined for samples of the Vermillion Creek coal bed and associated rocks in the Vermillion Creek basin and for samples of evaporites collected from Jurassic and Triassic formations that crop out in the nearby Uinta Mountains. The data are inconclusive, but it is likely that the sulfur in the coal was derived from the evaporites.

  16. Actinide Oxidation State and O/M Ratio in Hypostoichiometric Uranium-Plutonium-Americium U0.750Pu0.246Am0.004O2-x Mixed Oxides.

    PubMed

    Vauchy, Romain; Belin, Renaud C; Robisson, Anne-Charlotte; Lebreton, Florent; Aufore, Laurence; Scheinost, Andreas C; Martin, Philippe M

    2016-03-01

    Innovative americium-bearing uranium-plutonium mixed oxides U1-yPuyO2-x are envisioned as nuclear fuel for sodium-cooled fast neutron reactors (SFRs). The oxygen-to-metal (O/M) ratio, directly related to the oxidation state of cations, affects many of the fuel properties. Thus, a thorough knowledge of its variation with the sintering conditions is essential. The aim of this work is to follow the oxidation state of uranium, plutonium, and americium, and so the O/M ratio, in U0.750Pu0.246Am0.004O2-x samples sintered for 4 h at 2023 K in various Ar + 5% H2 + z vpm H2O (z = ∼ 15, ∼ 90, and ∼ 200) gas mixtures. The O/M ratios were determined by gravimetry, XAS, and XRD and evidenced a partial oxidation of the samples at room temperature. Finally, by comparing XANES and EXAFS results to that of a previous study, we demonstrate that the presence of uranium does not influence the interactions between americium and plutonium and that the differences in the O/M ratio between the investigated conditions is controlled by the reduction of plutonium. We also discuss the role of the homogeneity of cation distribution, as determined by EPMA, on the mechanisms involved in the reduction process. PMID:26907589

  17. Water isotopes in desiccating lichens

    PubMed Central

    Cuntz, Matthias; Máguas, Cristina; Lakatos, Michael

    2009-01-01

    The stable isotopic composition of water is routinely used as a tracer to study water exchange processes in vascular plants and ecosystems. To date, no study has focussed on isotope processes in non-vascular, poikilohydric organisms such as lichens and bryophytes. To understand basic isotope exchange processes of non-vascular plants, thallus water isotopic composition was studied in various green-algal lichens exposed to desiccation. The study indicates that lichens equilibrate with the isotopic composition of surrounding water vapour. A model was developed as a proof of concept that accounts for the specific water relations of these poikilohydric organisms. The approach incorporates first their variable thallus water potential and second a compartmentation of the thallus water into two isotopically distinct but connected water pools. Moreover, the results represent first steps towards the development of poikilohydric organisms as a recorder of ambient vapour isotopic composition. PMID:19888598

  18. Water isotopes in desiccating lichens.

    PubMed

    Hartard, Britta; Cuntz, Matthias; Máguas, Cristina; Lakatos, Michael

    2009-12-01

    The stable isotopic composition of water is routinely used as a tracer to study water exchange processes in vascular plants and ecosystems. To date, no study has focussed on isotope processes in non-vascular, poikilohydric organisms such as lichens and bryophytes. To understand basic isotope exchange processes of non-vascular plants, thallus water isotopic composition was studied in various green-algal lichens exposed to desiccation. The study indicates that lichens equilibrate with the isotopic composition of surrounding water vapour. A model was developed as a proof of concept that accounts for the specific water relations of these poikilohydric organisms. The approach incorporates first their variable thallus water potential and second a compartmentation of the thallus water into two isotopically distinct but connected water pools. Moreover, the results represent first steps towards the development of poikilohydric organisms as a recorder of ambient vapour isotopic composition. PMID:19888598

  19. Iron isotope biosignatures

    NASA Technical Reports Server (NTRS)

    Beard, B. L.; Johnson, C. M.; Cox, L.; Sun, H.; Nealson, K. H.; Aguilar, C.

    1999-01-01

    The (56)Fe/(54)Fe of Fe-bearing phases precipitated in sedimentary environments varies by 2.5 per mil (delta(56)Fe values of +0.9 to -1. 6 per mil). In contrast, the (56)Fe/(54)Fe of Fe-bearing phases in igneous rocks from Earth and the moon does not vary measurably (delta(56)Fe = 0.0 +/- 0.3 per mil). Experiments with dissimilatory Fe-reducing bacteria of the genus Shewanella algae grown on a ferrihydrite substrate indicate that the delta(56)Fe of ferrous Fe in solution is isotopically lighter than the ferrihydrite substrate by 1.3 per mil. Therefore, the range in delta(56)Fe values of sedimentary rocks may reflect biogenic fractionation, and the isotopic composition of Fe may be used to trace the distribution of microorganisms in modern and ancient Earth.

  20. Selenium isotope analysis

    SciTech Connect

    Webster, C.L. Jr.; Warren, C.G.

    1981-01-01

    The isotope ratio of selenium-80 to selenium-74 was determined on an isotope ratio mass spectrometer. Samples of 2 to 4 mg of selenium were fluorinated with CoF/sub 3/ in a small disposable copper bomb. The product, SeF/sub 6/, was purified in a vacuum line by distillation. The /sup 80/Se//sup 74/Se ratio was determined on a double-collector mass spectrometer that was modified to collect either /sup 82/Se-/sup 80/Se or /sup 80/Se-/sup 74/Se ion pairs. The standard deviation of the difference between two individually fluorinated samples was about 1 per mil. Because essentially all the error was associated with the fluorination step, comparisons between a standard of SeF/sub 6/ and individually fluorinated samples can be expected to have a standard deviation of about 0.5 per mil.

  1. New Isotope 263Hs

    SciTech Connect

    Dragojevic, I.; Gregorich, K.E.; Dullmann, Ch.E.; Dvorak, J.; Ellison, P.A.; Gates, J.M.; Nelson, S.L.; Stavsetra, L.; Nitsche, H.

    2010-03-16

    A new isotope of Hs was produced in the reaction 208Pb(56Fe, n)263Hs at the 88-Inch Cyclotron of the Lawrence Berkeley National Laboratory. Six genetically correlated nuclear decay chains have been observed and assigned to the new isotope 263Hs. The measured cross section was 21+13-8.4 pb at 276.4 MeV lab-frame center-of-target beam energy. 263Hs decays with a half-life of 0.74 ms by alpha-decay and the measured alpha-particle energies are 10.57 +- 0.06, 10.72 +- 0.06, and 10.89 +- 0.06 MeV. The experimental cross section is compared to a theoretical prediction based on the Fusion by Diffusion model [W. J. Swiatecki et al., Phys. Rev. C 71, 014602 (2005)].

  2. Isotope shift in chromium

    NASA Astrophysics Data System (ADS)

    Furmann, B.; Jarosz, A.; Stefańska, D.; Dembczyński, J.; Stachowska, E.

    2005-01-01

    Thirty-three spectral lines of chromium atom in the blue-violet region (425-465 nm) have been investigated with the method of laser-induced resonance fluorescence on an atomic beam. For all the lines, the isotope shifts for every pair of chromium isotopes have been determined. The lines can be divided into six groups, according to the configuration of the upper and lower levels. Electronic factors of the field shift and the specific mass shift ( Fik and MikSMS, respectively) have been evaluated and the values for each pure configuration involved have been determined. Comparison of the values Fik and MikSMS to the ab initio calculations results has been performed. The presence of crossed second order (CSO) effects has been observed.

  3. Isotope ratio analysis of actinides, fission products, and geolocators by high-efficiency multi-collector thermal ionization mass spectrometry

    NASA Astrophysics Data System (ADS)

    Bürger, S.; Riciputi, L. R.; Bostick, D. A.; Turgeon, S.; McBay, E. H.; Lavelle, M.

    2009-09-01

    A ThermoFisher "Triton" multi-collector thermal ionization mass spectrometer (MC-TIMS) was evaluated for trace and ultra-trace level isotope ratio analysis of actinides (uranium, plutonium, and americium), fission products and geolocators (strontium, cesium, and neodymium). Total efficiencies (atoms loaded to ions detected) of up to 0.5-2% for U, Pu, and Am, and 1-30% for Sr, Cs, and Nd can be reported employing resin bead load techniques onto flat ribbon Re filaments or resin beads loaded into a millimeter-sized cavity drilled into a Re rod. This results in detection limits of <0.1 fg (104 atoms to 105 atoms) for 239-242+244Pu, 233+236U, 241-243Am, 89,90Sr, and 134,135,137Cs, and <=1 pg for natural Nd isotopes (limited by the chemical processing blank) using a secondary electron multiplier (SEM) or multiple-ion counters (MICs). Relative standard deviations (RSD) as small as 0.1% and abundance sensitivities of 1 × 106 or better using a SEM are reported here. Precisions of RSD [approximate]0.01-0.001% using a multi-collector Faraday cup array can be achieved at sub-nanogram concentrations for strontium and neodymium and are suitable to gain crucial geolocation information. The analytical protocols reported herein are of particular value for nuclear forensic and nuclear safeguard applications.

  4. Stable isotope laser spectroscopy

    NASA Technical Reports Server (NTRS)

    Becker, J. F.; Yaldaei, Ramil; Mckay, Christopher P.

    1989-01-01

    Recent advances in semiconductor laser technology have produced a reliable lightweight device ideally suited for a spacecraft high resolution molecular spectrometer. Lead-salt tunable diode lasers (TDL) emit in several spectral modes, each with a very narrow linewidth of -0.0003/cm. This spectral resolution is much narrower than typical Doppler broadened molecular linewidths in the mid-IR range. Thus it is possible to detect individual rotational lines within the vibrational band and measure their intensity, which can be used to determine gas concentration. The narrow spectral lines of any impurity gas tend to lie between the narrow lines of the gas of interest. This represents a major advantage over the accepted gas chromatograph mass spectrometer (GCMS) technique for measuring gas concentrations and isotope ratios. The careful and extensive gas purification procedures required to remove impurities for reliable GCMS measurements will not be required for an IR laser gas analysis. The infrared laser gas analysis technique is being developed to measure stable isotopic ratios of gases such as CO2, CH4, N2O, and NH3. This will eventually lead to development of instruments capable of in situ istopic measurements on planets such as Mars. The carbon (C-12, C-13) isotope ratio is indicative of the type of carbon fixation mechanisms (e.g., photosynthesis, respiration) in operation on a planet, while the nitrogen (N-14, N-15) isotope ratio can probably be used to date nitrogen-bearing Martian samples. The absorbance ratio of two adjacent lines of CO2 in the 2300/cm (4.3 micron) region of the spectrum was measured. The precision of the measurement is presently better than 1 percent and significant improvement is anticipated as rapid sweep-integration techniques and computer controlled data acquistion capabilities are incorporated.

  5. Stable isotope laser spectroscopy

    NASA Astrophysics Data System (ADS)

    Becker, J. F.; Yaldaei, Ramil; McKay, Christopher P.

    1989-03-01

    Recent advances in semiconductor laser technology have produced a reliable lightweight device ideally suited for a spacecraft high resolution molecular spectrometer. Lead-salt tunable diode lasers (TDL) emit in several spectral modes, each with a very narrow linewidth of -0.0003/cm. This spectral resolution is much narrower than typical Doppler broadened molecular linewidths in the mid-IR range. Thus it is possible to detect individual rotational lines within the vibrational band and measure their intensity, which can be used to determine gas concentration. The narrow spectral lines of any impurity gas tend to lie between the narrow lines of the gas of interest. This represents a major advantage over the accepted gas chromatograph mass spectrometer (GCMS) technique for measuring gas concentrations and isotope ratios. The careful and extensive gas purification procedures required to remove impurities for reliable GCMS measurements will not be required for an IR laser gas analysis. The infrared laser gas analysis technique is being developed to measure stable isotopic ratios of gases such as CO2, CH4, N2O, and NH3. This will eventually lead to development of instruments capable of in situ istopic measurements on planets such as Mars. The carbon (C-12, C-13) isotope ratio is indicative of the type of carbon fixation mechanisms (e.g., photosynthesis, respiration) in operation on a planet, while the nitrogen (N-14, N-15) isotope ratio can probably be used to date nitrogen-bearing Martian samples. The absorbance ratio of two adjacent lines of CO2 in the 2300/cm (4.3 micron) region of the spectrum was measured. The precision of the measurement is presently better than 1 percent and significant improvement is anticipated as rapid sweep-integration techniques and computer controlled data acquistion capabilities are incorporated.

  6. ISOTOPE SEPARATING APPARATUS CONTROL

    DOEpatents

    Barnes, S.W.

    1959-08-25

    An improved isotope separating apparatus of the electromagnetic type, commonly referred to as a calutron, is described. Improvements in detecting and maintaining optimum position and focus of the ion beam are given. The calutron collector is provided with an additional electrode insulated from and positioned between the collecting pockets. The ion beams are properly positioned and focused until the deionizing current which flows from ground to this additional electrode ts a minimum.

  7. ISOTOPE METHODS IN HOMOGENEOUS CATALYSIS.

    SciTech Connect

    BULLOCK,R.M.; BENDER,B.R.

    2000-12-01

    The use of isotope labels has had a fundamentally important role in the determination of mechanisms of homogeneously catalyzed reactions. Mechanistic data is valuable since it can assist in the design and rational improvement of homogeneous catalysts. There are several ways to use isotopes in mechanistic chemistry. Isotopes can be introduced into controlled experiments and followed where they go or don't go; in this way, Libby, Calvin, Taube and others used isotopes to elucidate mechanistic pathways for very different, yet important chemistries. Another important isotope method is the study of kinetic isotope effects (KIEs) and equilibrium isotope effect (EIEs). Here the mere observation of where a label winds up is no longer enough - what matters is how much slower (or faster) a labeled molecule reacts than the unlabeled material. The most careti studies essentially involve the measurement of isotope fractionation between a reference ground state and the transition state. Thus kinetic isotope effects provide unique data unavailable from other methods, since information about the transition state of a reaction is obtained. Because getting an experimental glimpse of transition states is really tantamount to understanding catalysis, kinetic isotope effects are very powerful.

  8. Electrochemically controlled iron isotope fractionation

    NASA Astrophysics Data System (ADS)

    Black, Jay R.; Young, Edward D.; Kavner, Abby

    2010-02-01

    Variations in the stable isotope abundances of transition metals have been observed in the geologic record and trying to understand and reconstruct the physical/environmental conditions that produced these signatures is an area of active research. It is clear that changes in oxidation state lead to large fractionations of the stable isotopes of many transition metals such as iron, suggesting that transition metal stable isotope signatures could be used as a paleo-redox proxy. However, the factors contributing to these observed stable isotope variations are poorly understood. Here we investigate how the kinetics of iron redox electrochemistry generates isotope fractionation. Through a combination of electrodeposition experiments and modeling of electrochemical processes including mass-transport, we show that electron transfer reactions are the cause of a large isotope separation, while mass transport-limited supply of reactant to the electrode attenuates the observed isotopic fractionation. Furthermore, the stable isotope composition of electroplated transition metals can be tuned in the laboratory by controlling parameters such as solution chemistry, reaction overpotential, and solution convection. These methods are potentially useful for generating isotopically-marked metal surfaces for tracking and forensic purposes. In addition, our studies will help interpret stable isotope data in terms of identifying underlying electron transfer processes in laboratory and natural samples.

  9. Laser isotope separation of erbium and other isotopes

    DOEpatents

    Haynam, C.A.; Worden, E.F.

    1995-08-22

    Laser isotope separation is accomplished using at least two photoionization pathways of an isotope simultaneously, where each pathway comprises two or more transition steps. This separation method has been applied to the selective photoionization of erbium isotopes, particularly for the enrichment of {sup 167}Er. The hyperfine structure of {sup 167}Er was used to find two three-step photoionization pathways having a common upper energy level. 3 figs.

  10. Laser isotope separation of erbium and other isotopes

    DOEpatents

    Haynam, Christopher A.; Worden, Earl F.

    1995-01-01

    Laser isotope separation is accomplished using at least two photoionization pathways of an isotope simultaneously, where each pathway comprises two or more transition steps. This separation method has been applied to the selective photoionization of erbium isotopes, particularly for the enrichment of .sup.167 Er. The hyperfine structure of .sup.167 Er was used to find two three-step photoionization pathways having a common upper energy level.

  11. Oxygen isotope studies and compilation of isotopic dates from Antarctica

    SciTech Connect

    Grootes, P.M.; Stuiver, M.

    1986-01-01

    The Quaternary Isotope Laboratory, alone or in collaboration with other investigators, is currently involved in a number of oxygen-isotope studies mainly in Antarctica. Studies of a drill core from the South Pole, seasonal oxygen-18 signals preserved in the Dominion Range, isotope dating of the Ross Ice Shelf, oxygen-18 profiles of the Siple Coast, McMurdo Ice Shelf sampling, and a data compilation of radiometric dates from Antarctica are discussed.

  12. Nickel isotopes and methanogens

    NASA Astrophysics Data System (ADS)

    Neubeck, A.; Ivarsson, M.

    2013-12-01

    Methanogens require Ni for their growth and as a consequence the microbial fractionation of Ni isotopes can be used as a biomarker for activity of methanogenic communities1. Anaerobic laboratory experiments was performed using methanogens to investigate methanogenic growth in a modified nutrient media2 with olivine Fo91 (5g/l) added as an additional mineral nutrient source and as the only H2 provider. One of the investigated methanogens showed an increased growth in the experiments with added olivine. There were also a close relationship between the mobilized Ni and the growth of the methanogen. Ni is an element that previously has been neglected in the study of fossilized microorganisms and their interaction with mineral substrates and, thus, there are no records or published data of Ni in association with microfossils. However, we have detected enrichments of Ni in fossilized microorganisms and ichno-fossils, respectively, from three separate locations. Ni is not present in the host rock in any of the samples. Thus, Ni is present in association with fossilized microorganisms from environments and more extensive analysis is required to understand the magnitude, uptake, preservation and fractionation of Ni in microfossils. In order to analyze Ni isotope fractionation from microbe-mineral interaction, we plan to use a high-resolution Laser-Ablation Time-of-Flight Mass Spectrometer (LMS)3. In situ profile ablation will provide detailed and localized data on fractionation patterns between microfossils and their host rock. Also, this technique will allow us to identify the change in Ni isotopic fractionation in rock samples caused by abiotic and biogenic processes in a faster and easier way and with less risk for contamination compared to the wet chemistry analyses of Ni isotopes. 1. Cameron, V., Vance, D., Archer, C. & House, C. H. A biomarker based on the stable isotopes of nickel. Proceedings of the National Academy of Sciences 106, 10944-10948 (2009). 2. Schn

  13. Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution

    SciTech Connect

    Mincher, Bruce J.; Schmitt, Nicholas C.; Schuetz, Brian K.; Shehee, Thomas C.; Hobbs, David T.

    2015-03-11

    The peroxydisulfate anion has long been used for the preparation of hexavalent americium (AmVI) from the normally stable AmIII valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (AmV) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of AmVI. Incomplete oxidation would be expected to leave residual AmIII, or to produce AmV in treated solutions. However, until recently, the use of peroxydisulfate as an AmV reagent has not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative AmV was prepared in an acidic solution and the UV/Vis extinction coefficients of the AmV 513 nm peak were measured over a range of nitric acid concentrations. Furthermore, the utility of AmV for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers was also investigated.

  14. Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution.

    SciTech Connect

    Bruce J. Mincher; Nicholas C. Schmitt

    2015-03-01

    The peroxydisulfate anion has long been used for the preparation of hexavalent americium (AmVI) from the normally stable AmIII valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (AmV) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of AmVI. Incomplete oxidation would be expected to leave residual AmIII, or to produce AmV in treated solutions. However, until recently, the use of peroxydisulfate as an AmV reagent has not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative AmV was prepared in an acidic solution and the UV/Vis extinction coefficients of the AmV 513 nm peak were measured over a range of nitric acid concentrations. The utility of AmV for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers was also investigated.

  15. Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution

    DOE PAGESBeta

    Mincher, Bruce J.; Schmitt, Nicholas C.; Schuetz, Brian K.; Shehee, Thomas C.; Hobbs, David T.

    2015-03-11

    The peroxydisulfate anion has long been used for the preparation of hexavalent americium (AmVI) from the normally stable AmIII valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (AmV) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of AmVI. Incomplete oxidation would be expected to leave residual AmIII, or to produce AmV in treated solutions. However, until recently, the use of peroxydisulfate as an AmV reagent hasmore » not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative AmV was prepared in an acidic solution and the UV/Vis extinction coefficients of the AmV 513 nm peak were measured over a range of nitric acid concentrations. Furthermore, the utility of AmV for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers was also investigated.« less

  16. Laser Ablation Molecular Isotopic Spectrometry

    NASA Astrophysics Data System (ADS)

    Russo, Richard E.; Bol'shakov, Alexander A.; Mao, Xianglei; McKay, Christopher P.; Perry, Dale L.; Sorkhabi, Osman

    2011-02-01

    A new method of performing optical isotopic analysis of condensed samples in ambient air and at ambient pressure has been developed: Laser Ablation Molecular Isotopic Spectrometry (LAMIS). The technique uses radiative transitions from molecular species either directly vaporized from a sample or formed by associative mechanisms of atoms or ions in a laser ablation plume. This method is an advanced modification of a known atomic emission technique called laser-induced breakdown spectroscopy (LIBS). The new method — LAMIS — can determine not only chemical composition but also isotopic ratios of elements in the sample. Isotopic measurements are enabled by significantly larger isotopic shifts found in molecular spectra relative to atomic spectra. Analysis can be performed from a distance and in real time. No sample preparation or pre-treatment is required. Detection of the isotopes of hydrogen, boron, carbon, and oxygen are discussed to illustrate the technique.

  17. Isotopic anomalies in extraterrestrial grains.

    PubMed

    Ireland, T R

    1996-03-01

    Isotopic compositions are referred to as anomalous if the isotopic ratios measured cannot be related to the terrestrial (solar) composition of a given element. While small effects close to the resolution of mass spectrometric techniques can have ambiguous origins, the discovery of large isotopic anomalies in inclusions and grains from primitive meteorites suggests that material from distinct sites of stellar nucleosynthesis has been preserved. Refractory inclusions, which are predominantly composed of the refractory oxides of Al, Ca, Ti, and Mg, in chondritic meteorites commonly have excesses in the heaviest isotopes of Ca, Ti, and Cr which are inferred to have been produced in a supernova. Refractory inclusions also contain excess 26Mg from short lived 26Al decay. However, despite the isotopic anomalies indicating the preservation of distinct nucleosynthetic sites, refractory inclusions have been processed in the solar system and are not interstellar grains. Carbon (graphite and diamond) and silicon carbide grains from the same meteorites also have large isotopic anomalies but these phases are not stable in the oxidized solar nebula which suggests that they are presolar and formed in the circumstellar atmospheres of carbon-rich stars. Diamond has a characteristic signature enriched in the lightest and heaviest isotopes of Xe, and graphite shows a wide range in C isotopic compositions. SiC commonly has C and N isotopic signatures which are characteristic of H-burning in the C-N-O cycle in low-mass stars. Heavier elements such as Si, Ti, Xe, Ba, and Nd, carry an isotopic signature of the s-process. A minor population of SiC (known as Grains X, ca. 1%) are distinct in having decay products of short lived isotopes 26Al (now 26Mg), 44Ti (now 44Ca), and 49V (now 49Ti), as well as 28Si excesses which are characteristic of supernova nucleosynthesis. The preservation of these isotopic anomalies allows the examination of detailed nucleosynthetic pathways in stars. PMID

  18. ISOTOPE FRACTIONATION PROCESS

    DOEpatents

    Clewett, G.H.; Lee, DeW.A.

    1958-05-20

    A new method is described for isotopic enrichment of uranium. It has been found that when an aqueous acidic solution of ionic tetravalent uraniunn is contacted with chelate complexed tetravalent uranium, the U/sup 238/ preferentially concentrates in the complexed phase while U/sup 235/ concentrates in the ionic phase. The effect is enhanced when the chelate compound is water insoluble and is dissolved in a water-immiscible organic solvent. Cupferron is one of a number of sultable complexing agents, and chloroform is a suitable organic solvent.

  19. Tank waste isotope contributions

    SciTech Connect

    VANKEUREN, J.C.

    1999-08-26

    This document presents the results of a calculation to determine the relative contribution of selected isotopes to the inhalation and ingestion doses for a postulated release of Hanford tank waste. The fraction of the dose due to {sup 90}Sr, {sup 90}Y, {sup 137}Cs and the alpha emitters for single shell solids and liquids, double shell solids and liquids, aging waste solids and liquids and all solids and liquids. An effective dose conversion factor was also calculated for the alpha emitters for each composite of the tank waste.

  20. Chromatographic hydrogen isotope separation

    DOEpatents

    Aldridge, F.T.

    Intermetallic compounds with the CaCu/sub 5/ type of crystal structure, particularly LaNiCo/sub 4/ and CaNi/sub 5/, exhibit high separation factors and fast equilibrium times and therefore are useful for packing a chromatographic hydrogen isotope separation column. The addition of an inert metal to dilute the hydride improves performance of the column. A large scale multi-stage chromatographic separation process run as a secondary process off a hydrogen feedstream from an industrial plant which uses large volumes of hydrogen cn produce large quantities of heavy water at an effective cost for use in heavy water reactors.

  1. Chromatographic hydrogen isotope separation

    DOEpatents

    Aldridge, Frederick T.

    1981-01-01

    Intermetallic compounds with the CaCu.sub.5 type of crystal structure, particularly LaNiCo.sub.4 and CaNi.sub.5, exhibit high separation factors and fast equilibrium times and therefore are useful for packing a chromatographic hydrogen isotope separation colum. The addition of an inert metal to dilute the hydride improves performance of the column. A large scale mutli-stage chromatographic separation process run as a secondary process off a hydrogen feedstream from an industrial plant which uses large volumes of hydrogen can produce large quantities of heavy water at an effective cost for use in heavy water reactors.

  2. Quantitative Determination of Isotope Ratios from Experimental Isotopic Distributions

    PubMed Central

    Kaur, Parminder; O’Connor, Peter B.

    2008-01-01

    Isotope variability due to natural processes provides important information for studying a variety of complex natural phenomena from the origins of a particular sample to the traces of biochemical reaction mechanisms. These measurements require high-precision determination of isotope ratios of a particular element involved. Isotope Ratio Mass Spectrometers (IRMS) are widely employed tools for such a high-precision analysis, which have some limitations. This work aims at overcoming the limitations inherent to IRMS by estimating the elemental isotopic abundance from the experimental isotopic distribution. In particular, a computational method has been derived which allows the calculation of 13C/12C ratios from the whole isotopic distributions, given certain caveats, and these calculations are applied to several cases to demonstrate their utility. The limitations of the method in terms of the required number of ions and S/N ratio are discussed. For high-precision estimates of the isotope ratios, this method requires very precise measurement of the experimental isotopic distribution abundances, free from any artifacts introduced by noise, sample heterogeneity, or other experimental sources. PMID:17263354

  3. Mass-independent isotope effects.

    PubMed

    Buchachenko, Anatoly L

    2013-02-28

    Three fundamental properties of atomic nuclei-mass, spin (and related magnetic moment), and volume-are the source of isotope effects. The mostly deserved and popular, with almost hundred-year history, is the mass-dependent isotope effect. The first mass-independent isotope effect which chemically discriminates isotopes by their nuclear spins and nuclear magnetic moments rather than by their masses was detected in 1976. It was named as the magnetic isotope effect because it is controlled by magnetic interaction, i.e., electron-nuclear hyperfine coupling in the paramagnetic species, the reaction intermediates. The effect follows from the universal physical property of chemical reactions to conserve angular momentum (spin) of electrons and nuclei. It is now detected for oxygen, silicon, sulfur, germanium, tin, mercury, magnesium, calcium, zinc, and uranium in a great variety of chemical and biochemical reactions including those of medical and ecological importance. Another mass-independent isotope effect was detected in 1983 as a deviation of isotopic distribution in reaction products from that which would be expected from the mass-dependent isotope effect. On the physical basis, it is in fact a mass-dependent effect, but it surprisingly results in isotope fractionation which is incompatible with that predicted by traditional mass-dependent effects. It is supposed to be a function of dynamic parameters of reaction and energy relaxation in excited states of products. The third, nuclear volume mass-independent isotope effect is detected in the high-resolution atomic and molecular spectra and in the extraction processes, but there are no unambiguous indications of its importance as an isotope fractionation factor in chemical reactions. PMID:23301791

  4. ENVIRONMENTAL ISOTOPES FOR RESOLUTION OF HYDROLOGY PROBLEMS

    EPA Science Inventory

    The use of environmental isotopes as tracers in the hydrosphere is increasing as analytical instrumentation improves and more applications are discovered. There exists still misconceptions on the role of isotopes in resolving hydrology problems. Naturally occurring isotopes in th...

  5. Si Isotopes of Brownleeite

    NASA Technical Reports Server (NTRS)

    Nakamura-Messenger, K.; Messenger, Scott R.; Ito, M.; Keller, L. P.; Clemett, S. J.; Jones, J. H.; Tatsuoka, H.; Zolensky, M. E.; Tatsuoka, H.

    2010-01-01

    Brownleeite is a manganese silicide, ideally stoichiometric MnSi, not previously observed in nature until its discovery within an interplanetary dust particle (IDP) that likely originated from a comet [1]. Three discrete brownleeite grains in the IDP L2055 I3 (4 microns in size, hereafter IDP I3) were identified with maximum dimensions of 100, 250 and 600 nm and fully analyzed using scanning-transmission electron microscopy (STEM) [1]. One of the grains (100 nm in size) was poikilitically enclosed by low-Fe, Mn-enriched (LIME) olivine. LIME olivine is epitaxial to the brownleeite with the brownleeite (200) parallel to the olivine c* [1]. LIME olivine is an enigmatic phase first reported from chondritic porous IDPs and some unequilibrated ordinary chondrites [ 2], that is commonly observed in chondritic-porous IDPs. Recently, LIME olivine has been also found in comet Wild-2 (Stardust) samples [3], indicating that LIME olivine is a common mineral component of comets. LIME olivine has been proposed to form as a high temperature condensate in the protosolar nebula [2]. Brownleeite grains also likely formed as high-temperature condensates either in the early Solar System or in the outflow of an evolved star or supernova explosion [1]. The isotopic composition of the brownleeite grains may strongly constrain their ultimate source. To test this hypothesis, we performed isotopic analyses of the brownleeite and the associated LIME olivine, using the NASA/JSC NanoSIMS 50L ion microprobe.

  6. Phonon coherence in isotopic silicon superlattices

    SciTech Connect

    Frieling, R.; Radek, M.; Eon, S.; Bracht, H.; Wolf, D. E.

    2014-09-29

    Recent experimental and theoretical investigations have confirmed that a reduction in thermal conductivity of silicon is achieved by isotopic silicon superlattices. In the present study, non-equilibrium molecular dynamics simulations are performed to identify the isotope doping and isotope layer ordering with minimum thermal conductivity. Furthermore, the impact of isotopic intermixing at the superlattice interfaces on phonon transport is investigated. Our results reveal that the coherence of phonons in isotopic Si superlattices is prevented if interfacial mixing of isotopes is considered.

  7. Calcium isotopes in wine

    NASA Astrophysics Data System (ADS)

    Holmden, C. E.

    2011-12-01

    The δ 44/40Ca values of bottled wine vary between -0.76% to -1.55% on the seawater scale and correlate weakly with inverse Ca concentration and Mg/Ca ratio, such that the lowest δ 44/40Ca values have the highest Ca concentrations and lowest Mg/Ca ratios. The correlation is notable in the sense that the measured wines include both whites and reds sampled from different wine growing regions of the world, and cover a wide range of quality. Trends among the data yield clues regarding the cause of the observed isotopic fractionation. White wines, and wines generally perceived to be of lower quality, have lower δ 44/40Ca values compared to red wines and wines of generally perceived higher quality. Quality was assessed qualitatively through sensory evaluation, price, and scores assigned by critics. The relationship between δ 44/40Ca and wine quality was most apparent when comparing wines of one varietal from one producer from the same growing region. In the vineyard, wine quality is related to factors such as the tonnage of the crop and the ripeness of the grapes at the time of harvesting, the thickness of the skins for reds, the age of the vines, as well as the place where the grapes were grown (terroir). Quality is also influenced by winemaking practices such as fermentation temperature, duration of skin contact, and barrel ageing. Accordingly, the relationship between δ 44/40Ca and wine quality may originate during grape ripening in the vineyard or during winemaking in the cellar. We tested the grape ripening hypothesis using Merlot grapes sampled from a vineyard in the Okanagan, British Columbia, using sugar content (degrees Brix) as an indicator of ripeness. The grapes were separated into pulp, skin, and pip fractions and were analyzed separately. Thus far, there is no clear evidence for a systematic change in δ 44/40Ca values associated with progressive ripening of grapes in the vineyard. On the day of harvesting, the δ 44/40Ca value of juice squeezed from

  8. Aleutian terranes from Nd isotopes

    NASA Technical Reports Server (NTRS)

    Kay, R. W.; Kay, S. M.; Rubenstone, J. L.

    1986-01-01

    Nd isotope ratios substantiate the identification of oceanic crustal terranes within the continental crustal basement of the Aleutian island arc. The oceanic terranes are exposed in the westernmost Aleutians, but to the east, they are completely buried by isotopically distinct arc-volcanic rocks. Analogous oceanic terranes may be important components of the terrane collages that comprise the continents.

  9. The straight dope on isotopes

    NASA Astrophysics Data System (ADS)

    Thornton, Brett F.; Burdette, Shawn C.

    2013-12-01

    A century ago this month, Frederick Soddy described and named isotopes in the pages of Nature. Brett F. Thornton and Shawn C. Burdette discuss how chemists have viewed and used isotopes since then -- either as chemically identical or chemically distinct species as the need required and technology allowed.

  10. Method of separating boron isotopes

    DOEpatents

    Jensen, R.J.; Thorne, J.M.; Cluff, C.L.

    1981-01-23

    A method of boron isotope enrichment involving the isotope preferential photolysis of (2-chloroethenyl)-dichloroborane as the feed material. The photolysis can readily by achieved with CO/sub 2/ laser radiation and using fluences significantly below those required to dissociate BCl/sub 3/.

  11. Method of separating boron isotopes

    DOEpatents

    Jensen, Reed J.; Thorne, James M.; Cluff, Coran L.; Hayes, John K.

    1984-01-01

    A method of boron isotope enrichment involving the isotope preferential photolysis of (2-chloroethenyl)dichloroborane as the feed material. The photolysis can readily be achieved with CO.sub.2 laser radiation and using fluences significantly below those required to dissociate BCl.sub.3.

  12. Isotope separation by laser means

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

    1982-06-15

    A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

  13. Correlated optical and isotopic nanoscopy

    NASA Astrophysics Data System (ADS)

    Saka, Sinem K.; Vogts, Angela; Kröhnert, Katharina; Hillion, François; Rizzoli, Silvio O.; Wessels, Johannes T.

    2014-04-01

    The isotopic composition of different materials can be imaged by secondary ion mass spectrometry. In biology, this method is mainly used to study cellular metabolism and turnover, by pulsing the cells with marker molecules such as amino acids labelled with stable isotopes (15N, 13C). The incorporation of the markers is then imaged with a lateral resolution that can surpass 100 nm. However, secondary ion mass spectrometry cannot identify specific subcellular structures like organelles, and needs to be correlated with a second technique, such as fluorescence imaging. Here, we present a method based on stimulated emission depletion microscopy that provides correlated optical and isotopic nanoscopy (COIN) images. We use this approach to study the protein turnover in different organelles from cultured hippocampal neurons. Correlated optical and isotopic nanoscopy can be applied to a variety of biological samples, and should therefore enable the investigation of the isotopic composition of many organelles and subcellular structures.

  14. New insight into self-irradiation effects on local and long-range structure of uranium-americium mixed oxides (through XAS and XRD).

    PubMed

    Lebreton, Florent; Martin, Philippe M; Horlait, Denis; Bès, René; Scheinost, Andreas C; Rossberg, Andre; Delahaye, Thibaud; Blanchart, Philippe

    2014-09-15

    Uranium-americium mixed oxides could be used as transmutation targets to lower Am inventory in spent nuclear fuels. Due to (241)Am activity, these materials are subjected to α-self-irradiation which provokes crystallographic disorder. Previous studies on U-Am mixed oxides gave first insight into α-radiation tolerance of these compounds, but have never been carried out for more than a year, whereas these compounds might be stored up to a few years between fabrication and irradiation. In this work, we study effects of self-irradiation on the structure of U(1-x)Am(x)O(2±δ) solid solutions (x = 0.15 and 0.20) aged 3 to 4 years. Especially, X-ray diffraction and X-ray absorption spectroscopy are combined to observe these effects from both long-range and local perspectives. Results show that the fluorite-type structure of U-Am mixed oxides withstands (241)Am α-irradiation without major damage. Despite the increase of interatomic distances and crystallographic disorder observed during the first months of storage, the present results show that a steady state is then reached. Thus, no detrimental factors have been identified in this study in terms of structural damage for several-year storage of U(1-x)Am(x)O(2±δ) pellets before irradiation. Furthermore, comparison between long-range and local evolution suggests that α-self-irradiation-induced defects are mainly located in low-ordered domains. Based on literature data and present results, the steady state appears related to the equilibrium between radioinduced defect formation and material self-healing. PMID:25162209

  15. Container for hydrogen isotopes

    DOEpatents

    Solomon, David E.

    1977-01-01

    A container for the storage, shipping and dispensing of hydrogen isotopes such as hydrogen, deuterium, tritium, or mixtures of the same which has compactness, which is safe against fracture or accident, and which is reusable. The container consists of an outer housing with suitable inlet and outlet openings and electrical feed elements, the housing containing an activated sorber material in the form, for example, of titanium sponge or an activated zirconium aluminate cartridge. The gas to be stored is introduced into the chamber under conditions of heat and vacuum and will be retained in the sorber material. Subsequently, it may be released by heating the unit to drive off the stored gas at desired rates.

  16. Cometary Isotopic Measurements

    NASA Astrophysics Data System (ADS)

    Bockelée-Morvan, Dominique; Calmonte, Ursina; Charnley, Steven; Duprat, Jean; Engrand, Cécile; Gicquel, Adeline; Hässig, Myrtha; Jehin, Emmanuël; Kawakita, Hideyo; Marty, Bernard; Milam, Stefanie; Morse, Andrew; Rousselot, Philippe; Sheridan, Simon; Wirström, Eva

    2015-12-01

    Isotopic ratios in comets provide keys for the understanding of the origin of cometary material, and the physical and chemical conditions in the early Solar Nebula. We review here measurements acquired on the D/H, 14N/15N, 16O/18O, 12C/13C, and 32S/34S ratios in cometary grains and gases, and discuss their cosmogonic implications. The review includes analyses of potential cometary material available in collections on Earth, recent measurements achieved with the Herschel Space Observatory, large optical telescopes, and Rosetta, as well as recent results obtained from models of chemical-dynamical deuterium fractionation in the early solar nebula. Prospects for future measurements are presented.

  17. Lunar Surface Stirling Power Systems Using Isotope Heat Sources

    NASA Technical Reports Server (NTRS)

    Schmitz, Paul C.; Penswick, L. Barry; Shaltens, Richard K.

    2010-01-01

    For many years, NASA has used the decay of plutonium-238 (Pu-238) (in the form of the General Purpose Heat Source (GPHS)) as a heat source for Radioisotope Thermoelectric Generators (RTGs), which have provided electrical power for many NASA missions. While RTGs have an impressive reliability record for the missions in which they have been used, their relatively low thermal to electric conversion efficiency and the scarcity of plutonium-238 (Pu-238) has led NASA to consider other power conversion technologies. NASA is considering returning both robotic and human missions to the lunar surface and, because of the long lunar nights (14.75 Earth days), isotope power systems are an attractive candidate to generate electrical power. NASA is currently developing the Advanced Stirling Radioisotope Generator (ASRG) as a candidate higher efficiency power system that produces greater than 160 W with two GPHS modules at the beginning of life (BOL) (32% efficiency). The ASRG uses the same Pu-238 GPHS modules, which are used in RTG, but by coupling them to a Stirling convertor provides a four-fold reduction in the number of GPHS modules. This study considers the use of americium-241 (Am-241) as a substitute for the Pu-238 in Stirling- convertor-based Radioisotope Power Systems (RPS) for power levels from tens of watts to 5 kWe. The Am-241 is used as a substitute for the Pu-238 in GPHS modules. Depending on power level, different Stirling heat input and removal systems are modeled. It was found that substituting Am-241 GPHS modules into the ASRG reduces power output by about one-fifth while maintaining approximately the same system mass. In order to obtain the nominal 160 W of electrical output of the Pu-238 ASRG requires 10 Am-241 GPHS modules. Higher power systems require changing from conductive coupling heat input and removal from the Stirling convertor to either pumped loops or heat pipes. Liquid metal pumped loops are considered as the primary heat transportation on the hot

  18. Microbes: Agents of Isotopic Change

    NASA Astrophysics Data System (ADS)

    Fogel, M. L.

    2012-12-01

    Microbes drive many of the important oxidation and reduction reactions on Earth; digest almost all forms of organic matter; and can serve as both primary and secondary producers. Because of their versatile biochemistry and physiology, they impart unique isotopic signatures to organic and inorganic materials, which have proven to be key measurements for understanding elemental cycling now and throughout Earth's history. Understanding microbial isotope fractionations in laboratory experiments has been important for interpreting isotopic patterns measured in natural settings. In fact, the pairing of simple experiment with natural observation has been the pathway for interpreting the fingerprint of microbial processes in ancient sediments and rocks. Examples of how key experiments have explained stable isotope fractionations by microbes and advanced the field of microbial ecology will be presented. Learning the isotopic signatures of Earth's microbes is a valuable exercise for predicting what isotopic signatures could be displayed by possible extant or extinct extraterrestrial life. Given the potential for discovery on Mars, Enceladus, and other solar system bodies, new methods and techniques for pinpointing what is unique about microbial isotope signatures is particularly relevant.

  19. Isotopic analysis of planetary solids

    NASA Astrophysics Data System (ADS)

    Tulej, M.; Riedo, A.; Neuland, M.; Meyer, S.; Wurz, P.

    2013-09-01

    Isotopic analysis of planetary surfaces is of considerable interest for planetology. Studies of isotope composition can deliver information on radio-isotope chronology of planetary soil/regolith, an insight to processes that altered planetary surface (space weathering) or on possible biogenic processes that occurred or still occur on the planet. Mass spectrometry is a well-suited method that delivers accurate and precise isotope composition. Among other instruments (LAZMA and LAMS), the miniature laser ablation/ionisation mass analyser, LMS developed in Bern for in situ space research can be used to measure the elemental and isotopic composition of planetary solids. LMS support mass spectrometric investigation with a mass resolution of m/Δm≈500-1500, dynamic range of at least 8 decades and detection sensitivity of ~10 ppb. Current studies of various solid materials and standard reference materials show that isotope composition can be conducted with an accuracy and precision at per mill level if the isotope concentration exceeds 10-100 ppm. Implications of the studies for in situ application are discussed.

  20. Compelling Research Opportunities using Isotopes

    SciTech Connect

    2009-04-23

    Isotopes are vital to the science and technology base of the US economy. Isotopes, both stable and radioactive, are essential tools in the growing science, technology, engineering, and health enterprises of the 21st century. The scientific discoveries and associated advances made as a result of the availability of isotopes today span widely from medicine to biology, physics, chemistry, and a broad range of applications in environmental and material sciences. Isotope issues have become crucial aspects of homeland security. Isotopes are utilized in new resource development, in energy from bio-fuels, petrochemical and nuclear fuels, in drug discovery, health care therapies and diagnostics, in nutrition, in agriculture, and in many other areas. The development and production of isotope products unavailable or difficult to get commercially have been most recently the responsibility of the Department of Energy's Nuclear Energy program. The President's FY09 Budget request proposed the transfer of the Isotope Production program to the Department of Energy's Office of Science in Nuclear Physics and to rename it the National Isotope Production and Application program (NIPA). The transfer has now taken place with the signing of the 2009 appropriations bill. In preparation for this, the Nuclear Science Advisory Committee (NSAC) was requested to establish a standing subcommittee, the NSAC Isotope Subcommittee (NSACI), to advise the DOE Office of Nuclear Physics. The request came in the form of two charges: one, on setting research priorities in the short term for the most compelling opportunities from the vast array of disciplines that develop and use isotopes and two, on making a long term strategic plan for the NIPA program. This is the final report to address charge 1. NSACI membership is comprised of experts from the diverse research communities, industry, production, and homeland security. NSACI discussed research opportunities divided into three areas: (1) medicine

  1. Neodymium isotopic variations in seawater

    NASA Technical Reports Server (NTRS)

    Piepgras, D. J.; Wasserburg, G. J.

    1980-01-01

    Direct measurement of the isotopic composition of Nd in the Atlantic agree with the Nd content in ferromanganese sediments and differ from the observed amounts in the Pacific samples. These data indicate the existence of distinctive differences in the isotopic composition of Nd in the waters of major oceans; the average values determined from seawater and ferromanganese sediments are considerably lower than in sources with oceanic mantle affinities showing that the REE in the oceans is dominated by continental sources. The Nd isotopic variations in seawater are applied to relate the residence time of Nd and mixing rates between the oceans.

  2. Nucleon pairing in Sn isotopes

    NASA Astrophysics Data System (ADS)

    Imasheva, L.; Ishkhanov, B.; Stepanov, M.; Tretyakova, T.

    2016-01-01

    The systematics of excited states in Sn isotopes are discussed on basis of pairing interaction in nuclei. Nucleon paring leads to formation of excited states multiplets. The estimation of multiplet splitting based on experimental nuclear masses allows one to calculate the position of excited states with different seniority in δ-approximation. The wide systematics of the spectra of Sn isotopes gives a possibility to check the pairing interaction for different subshells and consider the multiplets of excited states in the neutron-rich isotopes far from stability.

  3. Carbon isotope geochemistry and geobiology

    NASA Technical Reports Server (NTRS)

    Desmarais, D.

    1985-01-01

    Carbon isotope fractionation values were used to understand the history of the biosphere. For example, plankton analyses confirmed that marine extinctions at the end of the Cretaceous period were indeed severe (see Hsu's article in Sundquist and Broeker, 1984). Variations in the isotopic compositions of carbonates and evaporitic sulfates during the Paleozoic reflect the relative abundances of euxinic (anoxic) marine environments and organic deposits from terrestrial flora. The carbon isotopic composition of Precambrian sediments suggest that the enzyme ribulose bisphosphate carboxylase has existed for perhaps 3.5 billion years.

  4. Magnesium isotopic composition of achondrites

    NASA Astrophysics Data System (ADS)

    Sedaghatpour, Fatemeh; Teng, Fang-Zhen

    2016-02-01

    Magnesium isotopic compositions of 22 well-characterized differentiated meteorites including 7 types of achondrites and pallasite meteorites were measured to estimate the average Mg isotopic composition of their parent bodies and evaluate Mg isotopic heterogeneity of the solar system. The δ26Mg values are -0.236‰ and -0.190‰ for acapulcoite-lodranite and angrite meteorites, respectively and vary from -0.267‰ to -0.222‰ in the winonaite-IAB-iron silicate group, -0.369‰ to -0.292‰ in aubrites, -0.269‰ to -0.158‰ in HEDs, -0.299‰ to -0.209‰ in ureilites, -0.307‰ to -0.237‰ in mesosiderites, and -0.303‰ to -0.238‰ in pallasites. Magnesium isotopic compositions of most achondrites and pallasite meteorites analyzed here are similar and reveal no significant isotopic fractionation. However, Mg isotopic compositions of D‧Orbigny (angrite) and some HEDs are slightly heavier than chondrites and the other achondrites studied here. The slightly heavier Mg isotopic compositions of angrites and some HEDs most likely resulted from either impact-induced evaporation or higher abundance of clinopyroxene with the Mg isotopic composition slightly heavier than olivine and orthopyroxene. The average Mg isotopic composition of achondrites (δ26Mg = -0.246 ± 0.082‰, 2SD, n = 22) estimated here is indistinguishable from those of the Earth (δ26Mg = -0.25 ± 0.07‰; 2SD, n = 139), chondrites (δ26Mg = -0.28 ± 0.06‰; 2SD, n = 38), and the Moon (δ26Mg = -0.26 ± 0.16‰; 2SD, n = 47) reported from the same laboratory. The chondritic Mg isotopic composition of achondrites, the Moon, and the Earth further reflects homogeneity of Mg isotopes in the solar system and the lack of Mg isotope fractionation during the planetary accretion process and impact events.

  5. Method for laser induced isotope enrichment

    DOEpatents

    Pronko, Peter P.; Vanrompay, Paul A.; Zhang, Zhiyu

    2004-09-07

    Methods for separating isotopes or chemical species of an element and causing enrichment of a desired isotope or chemical species of an element utilizing laser ablation plasmas to modify or fabricate a material containing such isotopes or chemical species are provided. This invention may be used for a wide variety of materials which contain elements having different isotopes or chemical species.

  6. Isotope separation using metallic vapor lasers

    NASA Technical Reports Server (NTRS)

    Russell, G. R.; Chen, C. J.; Harstad, K. G. (Inventor)

    1977-01-01

    The isotope U235 is separated from a gasified isotope mixture of U235 and U238 by selectively exciting the former from the ground state utilizing resonant absorption of radiation from precisely tuned lasers. The excited isotope is then selectively ionized by electron bombardment. It then is separated from the remaining isotope mixture by electromagnetic separation.

  7. Apparatus and process for separating hydrogen isotopes

    DOEpatents

    Heung, Leung K; Sessions, Henry T; Xiao, Xin

    2013-06-25

    The apparatus and process for separating hydrogen isotopes is provided using dual columns, each column having an opposite hydrogen isotopic effect such that when a hydrogen isotope mixture feedstock is cycled between the two respective columns, two different hydrogen isotopes are separated from the feedstock.

  8. Raman scattering method and apparatus for measuring isotope ratios and isotopic abundances

    DOEpatents

    Harney, Robert C.; Bloom, Stewart D.

    1978-01-01

    Raman scattering is used to measure isotope ratios and/or isotopic abundances. A beam of quasi-monochromatic photons is directed onto the sample to be analyzed, and the resulting Raman-scattered photons are detected and counted for each isotopic species of interest. These photon counts are treated mathematically to yield the desired isotope ratios or isotopic abundances.

  9. Isotope dilution mass spectrometry

    NASA Astrophysics Data System (ADS)

    Heumann, Klaus G.

    1992-09-01

    In the past isotope dilution mass spectrometry (IDMS) has usually been applied using the formation of positive thermal ions of metals. Especially in calibrating other analytical methods and for the certification of standard reference materials this type of IDMS became a routine method. Today, the progress in this field lies in the determination of ultra trace amounts of elements, e.g. of heavy metals in Antarctic ice and in aerosols in remote areas down to the sub-pg g-1 and sub-pg m-3 levels respectively, in the analysis of uranium and thorium at concentrations of a few pg g-1 in sputter targets for the production of micro- electronic devices or in the determination of sub-picogram amounts of230Th in corals for geochemical age determinations and of226Ra in rock samples. During the last few years negative thermal ionization IDMS has become a frequently used method. The determination of very small amounts of selenium and technetium as well as of other transition metals such as vanadium, chromium, molybdenum and tungsten are important examples in this field. Also the measurement of silicon in connection with a re-determination of Avogadro's number and osmium analyses for geological age determinations by the Re/Os method are of special interest. Inductively-coupled plasma mass spectrometry is increasingly being used for multi-element analyses by the isotope dilution technique. Determinations of heavy metals in samples of marine origin are representative examples for this type of multi-element analysis by IDMS. Gas chromatography-mass spectrometry systems have also been successfully applied after chelation of metals (for example Pt determination in clinical samples) or for the determination of volatile element species in the environment, e.g. dimethyl sulfide. However, IDMS--specially at low concentration levels in the environment--seems likely to be one of the most powerful analytical methods for speciation in the future. This has been shown, up to now, for species of

  10. Isotopic Analysis and Evolved Gases

    NASA Technical Reports Server (NTRS)

    Swindle, Timothy D.; Boynton, William V.; Chutjian, Ara; Hoffman, John H.; Jordan, Jim L.; Kargel, Jeffrey S.; McEntire, Richard W.; Nyquist, Larry

    1996-01-01

    Precise measurements of the chemical, elemental, and isotopic composition of planetary surface material and gases, and observed variations in these compositions, can contribute significantly to our knowledge of the source(s), ages, and evolution of solar system materials. The analyses discussed in this paper are mostly made by mass spectrometers or some other type of mass analyzer, and address three broad areas of interest: (1) atmospheric composition - isotopic, elemental, and molecular, (2) gases evolved from solids, and (3) solids. Current isotopic data on nine elements, mostly from in situ analysis, but also from meteorites and telescopic observations are summarized. Potential instruments for isotopic analysis of lunar, Martian, Venusian, Mercury, and Pluto surfaces, along with asteroid, cometary and icy satellites, surfaces are discussed.

  11. Isotopic Changes During Digestion: Protein

    NASA Astrophysics Data System (ADS)

    Tuross, N.

    2013-12-01

    Nutrient and hydrological inputs traverse a complicated route of pH, enzymatic and cellular processes in digestion in higher animals. The end products of digestion are the starting products for biosynthesis that are often used to interpret past life-ways. Using an artificial gut system, the isotopic changes (dD, d18O, d13C and d15N) of protein are documented. Three separate protein sources are subjected to the conditions, chemical and enzymatic, found in the stomach and upper small intestine with only a small shift in the oxygen isotopic composition of the proteins observed. Middle to lower small intestine parameters produced both greater isotopic effects and significantly lower molecular weight products. The role of the gastric enterocyte and the likely involvement of the internal milieu of this cell in the isotopic composition of amino acids that are transported to the liver are reported.

  12. Selective photoionisation of lutetium isotopes

    SciTech Connect

    D'yachkov, Aleksei B; Kovalevich, S K; Labozin, Valerii P; Mironov, Sergei M; Panchenko, Vladislav Ya; Firsov, Valerii A; Tsvetkov, G O; Shatalova, G G

    2012-10-31

    A three-stage laser photoionisation scheme intended for enriching the {sup 176}Lu isotope from natural lutetium was considered. An investigation was made of the hyperfine structure of the second excited state 5d6s7s {yields} {sup 4}D{sub 3/2} with an energy of 37194 cm{sup -1} and the autoionisation state with an energy of 53375 cm{sup -1} of the {sup 176}Lu and {sup 175}Lu isotopes. The total electron momentum of the autoionisation level and the constant A of hyperfine magnetic interaction were determined. Due to a small value of the isotopic shift between {sup 176}Lu and {sup 175}Lu, appreciable selectivity of their separation may be achieved with individual hyperfine structure components. The first tentative enrichment of the 176Lu isotope was performed to a concentration of 60 % - 70 %. (laser applications and other topics in quantum electronics)

  13. Titanium isotopic anomalies in meteorites

    NASA Astrophysics Data System (ADS)

    Neimeyer, S.; Lugmair, G. W.

    1984-07-01

    Studies of Ti isotopic compositions have shown that virtually every Ca-Al-rich Allende inclusion contains anomalous Ti. The present investigation is concerned with the results of a study of Ti isotopic compositions in meteorites. One objective of the study is to evaluate the possibility of a relation between oxygen and Ti anomalies, while another objective is to explore questions regarding the origin of the Ti anomalies. A summary of the major experimental findings of the study of Ti isotopic compositions is also presented. It is noted that an assessment of the implications of the Ti results favors a chemical memory type of model in which products from various nucleosynthetic sources survive in mineral grains. Isotopic heterogeneities are then preserved due to incomplete mixing and/or equilibriation with the bulk of solar system matter. Strong arguments are found to exist against a pure late supernova injection model.

  14. Physics with isotopically controlled semiconductors

    SciTech Connect

    Haller, E. E.

    2010-07-15

    This paper is based on a tutorial presentation at the International Conference on Defects in Semiconductors (ICDS-25) held in Saint Petersburg, Russia in July 2009. The tutorial focused on a review of recent research involving isotopically controlled semiconductors. Studies with isotopically enriched semiconductor structures experienced a dramatic expansion at the end of the Cold War when significant quantities of enriched isotopes of elements forming semiconductors became available for worldwide collaborations. Isotopes of an element differ in nuclear mass, may have different nuclear spins and undergo different nuclear reactions. Among the latter, the capture of thermal neutrons which can lead to neutron transmutation doping, is the most prominent effect for semiconductors. Experimental and theoretical research exploiting the differences in all the properties has been conducted and will be illustrated with selected examples.

  15. Titanium isotopic anomalies in meteorites

    NASA Technical Reports Server (NTRS)

    Niemeyer, S.; Lugmair, G. W.

    1984-01-01

    Studies of Ti isotopic compositions have shown that virtually every Ca-Al-rich Allende inclusion contains anomalous Ti. The present investigation is concerned with the results of a study of Ti isotopic compositions in meteorites. One objective of the study is to evaluate the possibility of a relation between oxygen and Ti anomalies, while another objective is to explore questions regarding the origin of the Ti anomalies. A summary of the major experimental findings of the study of Ti isotopic compositions is also presented. It is noted that an assessment of the implications of the Ti results favors a chemical memory type of model in which products from various nucleosynthetic sources survive in mineral grains. Isotopic heterogeneities are then preserved due to incomplete mixing and/or equilibriation with the bulk of solar system matter. Strong arguments are found to exist against a pure late supernova injection model.

  16. Clumped isotope thermometry and catagenesis

    NASA Astrophysics Data System (ADS)

    Eiler, J. M.; Clog, M. D.; Dallas, B.; Douglas, P. M.; Piasecki, A.; Sessions, A. L.; Stolper, D. A.

    2014-12-01

    Clumped- and site-specific isotopic compositions of organic compounds can constrain their formation temperatures, sources, and chemical reaction histories. The large number of isotopologues of organic molecules may allow for the isotopic composition of a single compound to illuminate many processes. For example, it is possible that clumping or site specific effects in different parts of the same molecule will differ in blocking temperature, such that a molecule's full isotopic structure could simultaneously constrain conditions of biosynthesis, catagenic 'cracking', and storage in the crust. Recent innovations in high-resolution mass spectrometry and methods of IR and NMR spectroscopy make it possible to explore these questions. Methane is the first organic molecule to have its clumped isotope geochemistry analyzed in a variety of natural environments and controlled experiments. Methane generated through catagenic cracking of kerogen and other organic matter forms in equilibrium with respect to isotopic clumping, and preserves that state through later storage or migration, up to temperatures of ~250 ˚C. This kinetic behavior permits a variety of useful geological applications. But it is unexpected because the bulk stable isotope composition of thermogenic methane is thought to reflect kinetic isotope effects on irreversible reactions. Our observations imply a new interpretation of the chemical physics of catagenic methane formation. Additional instrument and methods developments are currently extending the measurement of isotopic clumping and position specific effects to larger alkanes, other hydrocarbon compounds, and amino acids. These measurements will ultimately expand our capacity to understand the formational conditions and fates of organic molecules in high- and low-temperature environments through geological time.

  17. Isotope-Identifying neutron reflectometry

    SciTech Connect

    Nikitenko, Yu. V. Petrenko, A. V.; Gundorin, N. A.; Gledenov, Yu. M.; Aksenov, V. L.

    2015-07-15

    The possibilities of an isotope-indentifying study of layered structures in different regimes of a neutron wave field are considered. The detection of specularly reflected neutrons and secondary radiation (caused by neutron capture) in the form of charged particles, γ quanta, and nuclear fission fragments, as well as neutrons spin-flipped in a noncollinear magnetic field and on nuclei of elements with spin, makes it possible to implement isotope-indentifying neutron reflectometry.

  18. Novel hybrid isotope separation scheme and apparatus

    DOEpatents

    Maya, Jakob

    1991-01-01

    A method of yielding selectively a desired enrichment in a specific isotope including the steps of inputting into a spinning chamber a gas from which the specific isotope is to be isolated, radiating the gas with frequencies characteristic of the absorption of a particular isotope of the atomic or molecular gas, thereby inducing a photoionization reaction of the desired isotope, and collecting the specific isotope ion by suitable ion collection means.

  19. Novel hybrid isotope separation scheme and apparatus

    DOEpatents

    Maya, J.

    1991-06-18

    A method is described for yielding selectively a desired enrichment in a specific isotope including the steps of inputting into a spinning chamber a gas from which the specific isotope is to be isolated, radiating the gas with frequencies characteristic of the absorption of a particular isotope of the atomic or molecular gas, thereby inducing a photoionization reaction of the desired isotope, and collecting the specific isotope ion by suitable ion collection means. 3 figures.

  20. Impact of the cation distribution homogeneity on the americium oxidation state in the U0.54Pu0.45Am0.01O2-x mixed oxide

    NASA Astrophysics Data System (ADS)

    Vauchy, Romain; Robisson, Anne-Charlotte; Martin, Philippe M.; Belin, Renaud C.; Aufore, Laurence; Scheinost, Andreas C.; Hodaj, Fiqiri

    2015-01-01

    The impact of the cation distribution homogeneity of the U0.54Pu0.45Am0.01O2-x mixed oxide on the americium oxidation state was studied by coupling X-ray diffraction (XRD), electron probe micro analysis (EPMA) and X-ray absorption spectroscopy (XAS). Oxygen-hypostoichiometric Am-bearing uranium-plutonium mixed oxide pellets were fabricated by two different co-milling based processes in order to obtain different cation distribution homogeneities. The americium was generated from β- decay of 241Pu. The XRD analysis of the obtained compounds did not reveal any structural difference between the samples. EPMA, however, revealed a high homogeneity in the cation distribution for one sample, and substantial heterogeneity of the U-Pu (so Am) distribution for the other. The difference in cation distribution was linked to a difference in Am chemistry as investigated by XAS, with Am being present at mixed +III/+IV oxidation state in the heterogeneous compound, whereas only Am(IV) was observed in the homogeneous compound. Previously reported discrepancies on Am oxidation states can hence be explained by cation distribution homogeneity effects.

  1. Photo-induced isotopic fractionation

    NASA Astrophysics Data System (ADS)

    Miller, Charles E.; Yung, Yuk L.

    2000-12-01

    This paper presents a systematic method for the analysis of photo-induced isotopic fractionation. The physical basis for this fractionation mechanism centers on the fact that isotopic substitution alters the energy levels, molecular symmetries, spin statistical weights and other fundamental molecular properties, producing spectroscopic signatures distinguishable from that of the parent isotopomer. These mass-dependent physical properties are identical to those invoked by Urey to explain stable isotope fractionation in chemical systems subject to thermodynamic equilibrium. Photo-induced isotopic fractionation is a completely general phenomenon and should be observable in virtually all gas phase photochemical systems. Water photo-induced isotopic fractionation has been examined in detail using experimental and theoretical data. These results illustrate the salient features of this fractionation mechanism for molecules possessing continuous UV absorption spectra and unit photodissociation quantum yields. Using the photo-induced isotopic fractionation methodology in conjunction with standard photochemical models, we predict substantial deuterium enrichment of water vapor in the planetary atmospheres of Earth and Mars.

  2. Isotope separation apparatus and method

    DOEpatents

    Feldman, Barry J.

    1985-01-01

    The invention relates to an improved method and apparatus for laser isotope separation by photodeflection. A molecular beam comprising at least two isotopes to be separated intersects, preferably substantially perpendicular to one broad side of the molecular beam, with a laser beam traveling in a first direction. The laser beam is reflected back through the molecular beam, preferably in a second direction essentially opposite to the first direction. Because the molecules in the beam occupy various degenerate energy levels, if the laser beam comprises chirped pulses comprising selected wavelengths, the laser beam will very efficiently excite substantially all unexcited molecules and will cause stimulated emission of substantially all excited molecules of a selected one of the isotopes in the beam which such pulses encounter. Excitation caused by first direction chirped pulses moves molecules of the isotope excited thereby in the first direction. Stimulated emission of excited molecules of the isotope is brought about by returning chirped pulses traveling in the second direction. Stimulated emission moves emitting molecules in a direction opposite to the photon emitted. Because emitted photons travel in the second direction, emitting molecules move in the first direction. Substantial molecular movement of essentially all the molecules containing the one isotope is accomplished by a large number of chirped pulse-molecule interactions. A beam corer collects the molecules in the resulting enriched divergent portions of the beam.

  3. An ab initio study of the adsorption and dissociation of molecular oxygen on the (0 0 0 1) surface of double hexagonal close-packed americium

    NASA Astrophysics Data System (ADS)

    Dholabhai, Pratik P.; Atta-Fynn, Raymond; Ray, Asok K.

    2008-12-01

    In our continuing attempts to understand theoretically various surface properties such as corrosion and potential catalytic activity of actinide surfaces in the presence of environmental gases, we report here the first ab initio study of molecular adsorption on the double hexagonal close-packed (dhcp) americium (Am) (0 0 0 1) surface. Specifically, molecular oxygen adsorption on the (0 0 0 1) surface of dhcp Am has been studied in detail within the framework of density functional theory using a full-potential all-electron linearized augmented plane wave plus local orbitals (FP-LAPW+lo) method. Dissociative adsorption is found to be energetically more favorable compared to molecular adsorption. Chemisorption energies were optimized with respect to the distance of adsorbates from the surface for three approach positions at three adsorption sites, namely t1 (one-fold top), b2 (two-fold bridge), and h3 (three-fold hollow) sites. Chemisorption energies were computed at the scalar-relativistic-no-spin-orbit-coupling (SR-NSOC) and at the fully relativistic-with-spin-orbit-coupling (FR-SOC) levels of theory. The most stable configuration corresponds to a horizontal approach molecular dissociation with the oxygen atoms occupying neighboring h3 sites, with chemisorption energies at the NSOC and SOC theoretical levels being 9.395 and 9.886 eV, respectively. The corresponding distances of the oxygen molecule from the surface and oxygen-oxygen distance were found to be 0.953 and 3.731 Å, respectively. Overall our calculations indicate that chemisorption energies in cases with SOC are slightly more stable than those with NSOC in the 0.089-0.493 eV range. The work functions and net magnetic moments, respectively, increased and decreased in all cases compared to corresponding quantities of the bare dhcp-Am (0 0 0 1) surface. Adsorbate-substrate interactions have been analyzed in detail using partial charges inside muffin-tin spheres, difference charge density distributions, and

  4. Recovering Americium and Curium from Mark-42 Target Materials- New Processing Approaches to Enhance Separations and Integrate Waste Stream Disposition - 12228

    SciTech Connect

    Patton, Brad D.; Benker, Dennis; Collins, Emory D.; Mattus, Catherine H.; Robinson, Sharon M.; Wham, Robert M.

    2012-07-01

    Oak Ridge National Laboratory (ORNL) is investigating flowsheets to enhance processing efficiencies and to address waste streams associated with recovery of americium (Am) and curium (Cm) from Mark-42 (Mk-42) target materials stored at ORNL. The objective of this work was to identify the most effective flowsheet with which to process the 104 Mk-42 oxide capsules holding a total of 80 g of plutonium (Pu), 190 g of Cm, 480 g of Am, and 5 kg of lanthanide (Ln) oxides for the recovery and purification of the Am/Cm for future use as feedstock for heavy actinide production. Studies were also conducted to solidify the process flowsheet waste streams for disposal. ORNL is investigating flowsheets to enhance processing efficiencies and address waste streams associated with recovery of Am and Cm from Mk-42 target materials stored at ORNL. A series of small-scale runs are being performed to demonstrate an improved process to recover Am/Cm and to optimize the separations of Ln fission products from the Am/Cm constituents. The first of these runs has been completed using one of the Am/Cm/Ln oxide capsules stored at ORNL. The demonstration run showed promising results with a Ln DF of 40 for the Am/Cm product and an Am/Cm DF of 75 for the Ln product. In addition, the total losses of Am, Cm, and Ln to the waste solvents and raffinates were very low at <0.2%, 0.02%, and 0.04%, respectively. However, the Ln-actinide separation was less than desired. For future Reverse TALSPEAK demonstration runs, several parameters will be adjusted (flow rates, the ratio of scrub to strip stages, etc.) to improve the removal of Ln from the actinides. The next step will also include scale-up of the processing flowsheet to use more concentrated solutions (15 g/L Ln versus 5 g/L) and larger volumes and to recycle the HDEHP solvent. This should improve the overall processing efficiency and further reduce losses to waste streams. Studies have been performed with simulated wastes to develop solidification

  5. Isotopic Compositions of Evaporative Fluxes

    NASA Astrophysics Data System (ADS)

    Feng, X.; Lauder, A. M.; Kopec, B. G.; Dade, W. B.; Virginia, R. A.; Posmentier, E. S.

    2013-12-01

    The isotopic fluxes of evaporation from a water surface are typically computed using a one-dimensional model, originally conceptualized by Craig and Gordon (1965) and further developed and adapted to different natural settings (such as transpiration, open surface evaporation, etc.) by various investigators. These models have two distinguishing characteristics. First, there exists a laminar layer where molecular diffusion away from the water-air interface causes kinetic isotopic fractionation. The magnitude of this fractionation is controlled by the diffusion/transport coefficient of each vapor isotopologue in air and their concentration gradients, the latter being controlled by relative humidity, isotopic ratios of ambient air, and turbulent conditions (such as wind and surface roughness). Second, the horizontal variations are ignored. In particular, the effect of horizontal advection on isotopic variations in the ambient air is not considered. The research reported here addresses the effects of relinquishing the simplifying assumptions in both of these areas. We developed a model, in which the simplification of a purely laminar layer is dropped. Instead, we express the vertical transport coefficient as the sum of the molecular diffusivity, that differs for each water isotopologue, and the turbulent diffusivity that increases linearly with height but does not vary among water isotopologues. With this model, the kinetic isotopic effect reduces with height in the vicinity of the water surface, and the net isotopic fractionation through the boundary layer can be integrated. The advantage of this conceptualization is that the magnitude of kinetic isotopic fractionation can be assessed directly with changing environmental conditions, such as humidity and wind speed, rather than approximated by discontinuous empirical functions of the environmental conditions, as in the conventional models mentioned above. To address the effect of lateral heterogeneity, we expanded the

  6. Photodisintegration of Lithium Isotopes

    NASA Astrophysics Data System (ADS)

    Wurtz, Ward Andrew

    We have performed a measurement of the photodisintegration of the lithium isotopes, 6Li and 7Li, using a monochromatic, polarised photon beam and a segmented neutron detector array which covers approximately ¼ of 4pi srad. Using time-of-flight and scintillator light-output spectra we separate the data into individual reaction channels. This work is motivated by the need to compare with recent theoretical predictions and to provide data for future theoretical work. For the photodisintegration of 6Li we took data at 12 photon energies between 8 and 35 MeV. We describe the data using a model consisting of two-body reaction channels and obtain angular distributions and absolute cross sections for many of these reaction channels. We compare our results with a recent Lorentz integral transform calculation (Bacca et al. Phys. Rev. C 69, 057001 (2004)). Our results are in reasonable agreement with the calculation, in contradiction with previous experimental results. For the photodisintegration of 7Li, we took data at 9 photon energies between 10 and 35 MeV. We obtain cross sections for the reaction channel 7Li + gamma → n + 6 Li(g.s.) at all photon energies with angular distributions at all but the highest energy. We obtain angular distributions and total cross sections for reaction channels involving excited states of the daughter nucleus, 6Li, at select energies. We hope that these measurements will provide incentive for new theoretical calculations. We observe neutrons that can only be described by the reaction channel 7Li + gamma → n + 6Li(10.0) which necessitates an excited state of 6Li with excitation energy Ex = 10.0 +/- 0.5 MeV that is not in the standard tables of excited states. ii

  7. Isotope shifts in francium isotopes Fr-213206 and 221Fr

    NASA Astrophysics Data System (ADS)

    Collister, R.; Gwinner, G.; Tandecki, M.; Behr, J. A.; Pearson, M. R.; Zhang, J.; Orozco, L. A.; Aubin, S.; Gomez, E.; FrPNC Collaboration

    2014-11-01

    We present the isotope shifts of the 7 s1 /2 to 7 p1 /2 transition for francium isotopes 206 -213Fr with reference to 221Fr collected from two experimental periods. The shifts are measured on a sample of atoms prepared within a magneto-optical trap by a fast sweep of radio-frequency sidebands applied to a carrier laser. King plot analysis, which includes literature values for 7 s1 /2 to 7 p3 /2 isotope shifts, provides a field shift constant ratio of 1.0520(10) and a difference between the specific mass shift constants of 170(100) GHz amu between the D1 and D2 transitions, of sufficient precision to differentiate between ab initio calculations.

  8. Isotope separation apparatus and method

    DOEpatents

    Cotter, Theodore P.

    1982-12-28

    The invention relates to a method and apparatus for laser isotope separation by photodeflection. A molecular beam comprising at least two isotopes to be separated intersects, preferable substantially perpendicular to one broad side of the molecular beam, with a laser beam traveling in a first direction. The laser beam is reflected back through the molecular beam, preferably in a second direction essentially opposite to the first direction. The laser beam comprises .pi.-pulses of a selected wavelength which excite unexcited molecules, or cause stimulated emission of excited molecules of one of the isotopes. Excitation caused by first direction .pi.-pulses moves molecules of the isotope excited thereby in the first direction. Stimulated emission of excited molecules of the isotope is brought about by returning .pi.-pulses traveling in the second direction. Stimulated emission moves emitting molecules in a direction opposite to the photon emitted. Because emitted photons travel in the second direction, emitting molecules move in the first direction. Substantial molecular movement is accomplished by a large number of .pi.-pulse-molecule interactions. A beam corer collects the molecules in the resulting enriched divergent portions of the beam.

  9. Isotopic Randomness and Maxwell's Demon

    NASA Astrophysics Data System (ADS)

    Berezin, Alexander A.

    2005-03-01

    Isotopic disorder in crystals can lead to suppression of thermal conductivity, mobility variations and (weak) Anderson localization on isotopic fluctuations. The latter (AAB, J.ChemPhys.1984) is akin to polaron effect (self-localization due polarization). Possibility of isotopic patterning (IP) increases near melting point (thermally activated isotopic hopping swaps). Crystal near melting threshold become “informationally sensitive” as if its IP is operated by some external Maxwell’s Demon, MD (AAB, URAM J, 2002). At this state short range (e.g. electrostatic inverse square) forces evolve into long-range interactions (due to divergence of order parameter) and information sensitivity can be further amplified by (say) a single fast electron (e.g. beta-particle from decay of 14-C or other radioactive isotope) which may result in cascade of impact ionization events and (short time-scale) enhancement of screening by impact-generated non-equilibrium (non-thermal) electrons. In this state informationally driven (MD-controlled) IP (Eccles effect) can result in decrease of positional entropy signifying emergence of physical complexity out of pure information, similar to peculiar “jinni effect” on closed time loops in relativistic cosmology (R.J.Gott, 2001) or Wheeler’s “it from bit” metaphor. By selecting special IP, MD modifies ergodicity principle in favor of info rich states.

  10. Opportunities for isotope discoveries at FRIB

    NASA Astrophysics Data System (ADS)

    Baumann, T.; Hausmann, M.; Sherrill, B. M.; Tarasov, O. B.

    2016-06-01

    Expected production yields of the Facility for Rare Isotope Beams (FRIB) were calculated for a wide range of rare isotopes using the code LISE++ and planned performance parameters (Tarasov and Bazin, 2008; Bollen et al., 2011 [2]). A comparison between isotope discoveries of the last decade and expected particle yields indicates the range of isotopes that can likely be detected at FRIB. This paper will highlight recent isotope discoveries at NSCL's Coupled Cyclotron Facility and deduce how far the limits could be pushed with the Facility for Rare Isotope Beams.

  11. Isotope specific arbitrary material sorter

    SciTech Connect

    Barty, Christopher P.J.

    2015-12-08

    A laser-based mono-energetic gamma-ray source is used to provide a rapid and unique, isotope specific method for sorting materials. The objects to be sorted are passed on a conveyor in front of a MEGa-ray beam which has been tuned to the nuclear resonance fluorescence transition of the desired material. As the material containing the desired isotope traverses the beam, a reduction in the transmitted MEGa-ray beam occurs. Alternately, the laser-based mono-energetic gamma-ray source is used to provide non-destructive and non-intrusive, quantitative determination of the absolute amount of a specific isotope contained within pipe as part of a moving fluid or quasi-fluid material stream.

  12. Photonuclear reactions on titanium isotopes

    SciTech Connect

    Belyshev, S. S.; Dzhilavyan, L. Z.; Ishkhanov, B. S.; Kapitonov, I. M.; Kuznetsov, A. A. Orlin, V. N.; Stopani, K. A.

    2015-03-15

    The photodisintegration of titanium isotopes in the giant-dipole-resonance energy region is studied by the photon-activation method. Bremsstrahlung photons whose spectrum has the endpoint energy of 55 MeV is used. The yields and integrated cross sections are determined for photoproton reactions on the titanium isotopes {sup 47,48,49,50}Ti. The respective experimental results are compared with their counterparts calculated on the basis of the TALYS code and a combined photonucleon-reaction model. The TALYS code disregards the isospin structure of the giant dipole resonance and is therefore unable to describe the yield of photoproton reactions on the heavy titanium isotopes {sup 49,50}Ti.

  13. The terrestrial uranium isotope cycle

    NASA Astrophysics Data System (ADS)

    Andersen, Morten B.; Elliott, Tim; Freymuth, Heye; Sims, Kenneth W. W.; Niu, Yaoling; Kelley, Katherine A.

    2015-01-01

    Changing conditions on the Earth's surface can have a remarkable influence on the composition of its overwhelmingly more massive interior. The global distribution of uranium is a notable example. In early Earth history, the continental crust was enriched in uranium. Yet after the initial rise in atmospheric oxygen, about 2.4 billion years ago, the aqueous mobility of oxidized uranium resulted in its significant transport to the oceans and, ultimately, by means of subduction, back to the mantle. Here we explore the isotopic characteristics of this global uranium cycle. We show that the subducted flux of uranium is isotopically distinct, with high 238U/235U ratios, as a result of alteration processes at the bottom of an oxic ocean. We also find that mid-ocean-ridge basalts (MORBs) have 238U/235U ratios higher than does the bulk Earth, confirming the widespread pollution of the upper mantle with this recycled uranium. Although many ocean island basalts (OIBs) are argued to contain a recycled component, their uranium isotopic compositions do not differ from those of the bulk Earth. Because subducted uranium was probably isotopically unfractionated before full oceanic oxidation, about 600 million years ago, this observation reflects the greater antiquity of OIB sources. Elemental and isotope systematics of uranium in OIBs are strikingly consistent with previous OIB lead model ages, indicating that these mantle reservoirs formed between 2.4 and 1.8 billion years ago. In contrast, the uranium isotopic composition of MORB requires the convective stirring of recycled uranium throughout the upper mantle within the past 600 million years.

  14. The terrestrial uranium isotope cycle.

    PubMed

    Andersen, Morten B; Elliott, Tim; Freymuth, Heye; Sims, Kenneth W W; Niu, Yaoling; Kelley, Katherine A

    2015-01-15

    Changing conditions on the Earth's surface can have a remarkable influence on the composition of its overwhelmingly more massive interior. The global distribution of uranium is a notable example. In early Earth history, the continental crust was enriched in uranium. Yet after the initial rise in atmospheric oxygen, about 2.4 billion years ago, the aqueous mobility of oxidized uranium resulted in its significant transport to the oceans and, ultimately, by means of subduction, back to the mantle. Here we explore the isotopic characteristics of this global uranium cycle. We show that the subducted flux of uranium is isotopically distinct, with high (238)U/(235)U ratios, as a result of alteration processes at the bottom of an oxic ocean. We also find that mid-ocean-ridge basalts (MORBs) have (238)U/(235)U ratios higher than does the bulk Earth, confirming the widespread pollution of the upper mantle with this recycled uranium. Although many ocean island basalts (OIBs) are argued to contain a recycled component, their uranium isotopic compositions do not differ from those of the bulk Earth. Because subducted uranium was probably isotopically unfractionated before full oceanic oxidation, about 600 million years ago, this observation reflects the greater antiquity of OIB sources. Elemental and isotope systematics of uranium in OIBs are strikingly consistent with previous OIB lead model ages, indicating that these mantle reservoirs formed between 2.4 and 1.8 billion years ago. In contrast, the uranium isotopic composition of MORB requires the convective stirring of recycled uranium throughout the upper mantle within the past 600 million years. PMID:25592542

  15. Development of an "Isotopic" Pulser

    SciTech Connect

    Luke, S J; Schmid, G; Beckedahl, D; Pohl, B; White, G

    2002-06-04

    We have developed a pulser that is able to generate a simulated signal from a high-purity germanium (HPGe) detector for various plutonium isotopes. In this paper we describe the development of an ''isotopics'' pulser for the simulation of signals that are produced by an HPGe detector. The present pulser generates the waveforms that are produced by an HPGe detector both before and after the preamplifier. These signals have been input into a normal MCA and the result closely simulates a genuine pulse-height distribution.

  16. Feasibility of Isotopic Measurements: Graphite Isotopic Ratio Method

    SciTech Connect

    Wood, Thomas W.; Gerlach, David C.; Reid, Bruce D.; Morgan, W. C.

    2001-04-30

    This report addresses the feasibility of the laboratory measurements of isotopic ratios for selected trace constituents in irradiated nuclear-grade graphite, based on the results of a proof-of-principal experiment completed at Pacific Northwest National Laboratory (PNNL) in 1994. The estimation of graphite fluence through measurement of isotopic ratio changes in the impurity elements in the nuclear-grade graphite is referred to as the Graphite Isotope Ratio Method (GIRM). Combined with reactor core and fuel information, GIRM measurements can be employed to estimate cumulative materials production in graphite moderated reactors. This report documents the laboratory procedures and results from the initial measurements of irradiated graphite samples. The irradiated graphite samples were obtained from the C Reactor (one of several production reactors at Hanford) and from the French G-2 Reactor located at Marcoule. Analysis of the irradiated graphite samples indicated that replicable measurements of isotope ratios could be obtained from the fluence sensitive elements of Ti, Ca, Sr, and Ba. While these impurity elements are present in the nuclear-grade graphite in very low concentrations, measurement precision was typically on the order of a few tenths of a percent to just over 1 percent. Replicability of the measurements was also very good with measured values differing by less than 0.5 percent. The overall results of this initial proof-of-principal experiment are sufficiently encouraging that a demonstration of GIRM on a reactor scale basis is planned for FY-95.

  17. Phonon properties of americium phosphide

    NASA Astrophysics Data System (ADS)

    Arya, B. S.; Aynyas, Mahendra; Sanyal, S. P.

    2016-05-01

    Phonon properties of AmP have been studied by using breathing shell models (BSM) which includes breathing motion of electrons of the Am atoms due to f-d hybridization. The phonon dispersion curves, specific heat calculated from present model. The calculated phonon dispersion curves of AmP are presented follow the same trend as observed in uranium phosphide. We discuss the significance of this approach in predicting the phonon dispersion curves of these compounds and examine the role of electron-phonon interaction.

  18. Oxygen and silicon isotopes in ALHA 81005

    NASA Astrophysics Data System (ADS)

    Mayeda, T. K.; Clayton, R. N.; Molini-Velsko, C. A.

    1983-09-01

    The Antarctic meteorite ALHA81005 has oxygen and silicon isotopic compositions identical with lunar highland rocks. The oxygen is distinctly unlike that in calcium-rich achondrites. The isotopic data are entirely consistent with a lunar origin for the meteorite.

  19. Cosmology: Rare isotopic insight into the Universe

    NASA Astrophysics Data System (ADS)

    Prantzos, Nikos

    2016-01-01

    Light isotopes of hydrogen and helium formed minutes after the Big Bang. The study of one of these primordial isotopes, helium-3, has now been proposed as a useful strategy for constraining the physics of the standard cosmological model.

  20. Isotopic microanalysis of returned comet nucleus samples

    NASA Technical Reports Server (NTRS)

    Zinner, Ernst

    1989-01-01

    If isotopic measurements of interplanetary dust particles (IDPs) and primitive meteorites can serve as a guide to the isotopic analysis of returned comet nucleus material, an essential requirement will be the capability for microanalysis. The reason is that in both types of extraterrestrial samples large isotopic heterogeneities on a small spatial scale have become apparent once it was possible to measure isotopes in small samples. In the discovery of large isotopic anomalies the ion microprobe has played a significant role because of its high spatial resolution for isotopic ratio measurements. The largest isotopic anomalies in C, N, O, Mg, Si, Ca and Ti found to date were measured by ion microprobe mass spectrometry. The most striking examples are D/H measurements in IDPs and isotopic measurements of C, N and Si in SiC from the CM chondrites Murray and Murchison.

  1. APPLICATIONS OF ENVIRONMENTAL ISOTOPES FOR WATERSHED INVESTIGATIONS

    EPA Science Inventory

    Environmental isotopes include naturally-occurring nuclides that can be applied as tracers within watersheds (Sidle, 1998). Recent advances in mass spectroscopy may supplant many traditional and costly hydrometric techniques. It is now possible, for example, to utilize isotopes a...

  2. Online Catalog of Isotope Products from DOE's National Isotope Development Center

    DOE Data Explorer

    The National Isotope Development Center (NIDC) interfaces with the User Community and manages the coordination of isotope production across the facilities and business operations involved in the production, sale, and distribution of isotopes. A virtual center, the NIDC is funded by the Isotope Development and Production for Research and Applications (IDPRA) subprogram of the Office of Nuclear Physics in the U.S. Department of Energy Office of Science. The Isotope subprogram supports the production, and the development of production techniques of radioactive and stable isotopes that are in short supply for research and applications. Isotopes are high-priority commodities of strategic importance for the Nation and are essential for energy, medical, and national security applications and for basic research; a goal of the program is to make critical isotopes more readily available to meet domestic U.S. needs. This subprogram is steward of the Isotope Production Facility (IPF) at Los Alamos National Laboratory (LANL), the Brookhaven Linear Isotope Producer (BLIP) facility at BNL, and hot cell facilities for processing isotopes at ORNL, BNL and LANL. The subprogram also coordinates and supports isotope production at a suite of university, national laboratory, and commercial accelerator and reactor facilities throughout the Nation to promote a reliable supply of domestic isotopes. The National Isotope Development Center (NIDC) at ORNL coordinates isotope production across the many facilities and manages the business operations of the sale and distribution of isotopes.

  3. Separating Isotopes With Laser And Electron Beams

    NASA Technical Reports Server (NTRS)

    Trajmar, Sandor

    1989-01-01

    Need for second laser eliminated. In scheme for separation of isotopes, electrons of suitable kinetic energy ionize specific isotope excited by laser beam in magnetic field. Ionization by electron beams cheap and efficient in comparison to ionization by laser beams, and requires no special technical developments. Feasibility of new scheme demonstrated in selective ionization of Ba138, making possible separation of isotope from Ba isotopes of atomic weight 130, 132, 134, 135, 136, and 137.

  4. ICP-MS for isotope ratio measurement

    Technology Transfer Automated Retrieval System (TEKTRAN)

    The use of stable isotopes in mineral nutrition research has become a fundamental aspect of conducting this research. A gradual transition has occurred, now virtually complete, from radioactive isotope studies to those using stable isotopes. Although primarily used in human research, mineral stable ...

  5. Isotope Cancer Treatment Research at LANL

    SciTech Connect

    Weidner, John; Nortier, Meiring

    2012-04-11

    Los Alamos National Laboratory has produced medical isotopes for diagnostic and imaging purposes for more than 30 years. Now LANL researchers have branched out into isotope cancer treatment studies. New results show that an accelerator-based approach can produce clinical trial quantities of actinium-225, an isotope that has promise as a way to kill tumors without damaging surrounding healthy cells.

  6. Substitution of stable isotopes in Chlorella

    NASA Technical Reports Server (NTRS)

    Flaumenhaft, E.; Katz, J. J.; Uphaus, R. A.

    1969-01-01

    Replacement of biologically important isotopes in the alga Chlorella by corresponding heavier stable isotopes produces increasingly greater deviations from the normal cell size and changes the quality and distribution of certain cellular components. The usefulness of isotopically altered organisms increases interest in the study of such permuted organisms.

  7. Isotope Cancer Treatment Research at LANL

    ScienceCinema

    Weidner, John; Nortier, Meiring

    2014-06-02

    Los Alamos National Laboratory has produced medical isotopes for diagnostic and imaging purposes for more than 30 years. Now LANL researchers have branched out into isotope cancer treatment studies. New results show that an accelerator-based approach can produce clinical trial quantities of actinium-225, an isotope that has promise as a way to kill tumors without damaging surrounding healthy cells.

  8. Dry phase reactor for generating medical isotopes

    DOEpatents

    Mackie, Thomas Rockwell; Heltemes, Thad Alexander

    2016-05-03

    An apparatus for generating medical isotopes provides for the irradiation of dry-phase, granular uranium compounds which are then dissolved in a solvent for separation of the medical isotope from the irradiated compound. Once the medical isotope is removed, the dissolved compound may be reconstituted in dry granular form for repeated irradiation.

  9. Isotopic Fractionation in Interstellar Chemistry

    NASA Technical Reports Server (NTRS)

    Charnley, Steven

    2009-01-01

    Isotopically fractionated material is found in many solar system objects, including meteorites and comets. It is thought, in some cases, to trace interstellar material that was incorporated into the solar sys tem without undergoing significant processing. In this poster, we sho w the results of several models of the nitrogen, oxygen, and carbon f ractionation in proto-stellar cores.

  10. A NICHE FOR ISOTOPIC ECOLOGY

    EPA Science Inventory

    Fifty years ago, GE Hutchinson defined the ecological niche as a hypervolume in n-dimensional space with environmental variables as axes. Ecologists have recently developed renewed interest in the concept, and technological advances now allow us to use stable isotope analyses to ...

  11. Bayesian stable isotope mixing models

    EPA Science Inventory

    In this paper we review recent advances in Stable Isotope Mixing Models (SIMMs) and place them into an over-arching Bayesian statistical framework which allows for several useful extensions. SIMMs are used to quantify the proportional contributions of various sources to a mixtur...

  12. Isotope separation by laser technology

    NASA Astrophysics Data System (ADS)

    Stoll, Wolfgang

    2002-03-01

    Isotope separation processes operate on very small differences, given either by the Quotient of masses with the same number of electrons or by their mass difference. When separating isotopes of light elements in mass quantities, thermodynamic processes accounting for the quotient, either in diffusion, chemical reactivity or distillation are used. For heavy elements those quotients are very small. Therefore they need a large number of separation steps. Large plants with high energy consumption result from that. As uranium isotope separation is the most important industrial field, alternatives, taking account for the mass difference, as e.g. gas centrifuges, have been developed. They use only a fraction of the energy input, but need a very large number of machines, as the individual throughput is small. Since it was discovered, that molecules of high symmetry like Uranium-Hexafluoride as a deep-cooled gas stream can be ionized by multiple photon excitation, this process was studied in detail and in competition to the selective ionization of metal vapors, as already demonstrated with uranium. The paper reports about the principles of the laser excitation for both processes, the different laboratory scale and prototypical plants built, the difficulties with materials, as far as the metal vapor laser separation is concerned, and the difficulties experienced in the similarity in molecular spectra. An overview of the relative economic merits of the different processes and the auspices in a saturated market for uranium isotope separation, together with other potential markets for molecular laser separation, is contained in the conclusions.

  13. Isotope geochemistry in 1990s

    SciTech Connect

    Billo, S.M.

    1995-12-31

    The intense interest in radioactive minerals as a source of atomic energy, and their application in searching for ore deposits and also in gamma-ray and neutron logging oil wells, have opened new vistas in every science. Many minerals containing elements of high atomic weight are radioactive, and emit a radiation which affects a photographic plate and may be detected by means of a sensitive phosphorescent screen. Most of the elements as found in nature are a mixture of isotopes. isotopes are atoms of one element which have different masses. Uranium, thorium, potassium, and rubidium isotopes are also used to date minerals and rocks. Organic materials that have been in equilibrium with CO{sub 2}-photosynthetic cycle during the past 50,000 years are dated by carbon-14 method. The stable isotopes of H{sub 2}, C, N{sub 2}, O{sub 2}, and S are intimately associated with the atmosphere, hydrosphere, and lithosphere and are used in probing water resources.

  14. Deformation properties of lead isotopes

    NASA Astrophysics Data System (ADS)

    Tolokonnikov, S. V.; Borzov, I. N.; Lutostansky, Yu. S.; Saperstein, E. E.

    2016-01-01

    The deformation properties of a long lead isotopic chain up to the neutron drip line are analyzed on the basis of the energy density functional (EDF) in the FaNDF0 Fayans form. The question of whether the ground state of neutron-deficient lead isotopes can have a stable deformation is studied in detail. The prediction of this deformation is contained in the results obtained on the basis of the HFB-17 and HFB-27 Skyrme EDF versions and reported on Internet. The present analysis reveals that this is at odds with experimental data on charge radii and magnetic moments of odd lead isotopes. The Fayans EDF version predicts a spherical ground state for all light lead isotopes, but some of them (for example, 180Pb and 184Pb) prove to be very soft—that is, close to the point of a phase transition to a deformed state. Also, the results obtained in our present study are compared with the predictions of some other Skyrme EDF versions, including SKM*, SLy4, SLy6, and UNE1. By and large, their predictions are closer to the results arising upon the application of the Fayans functional. For example, the SLy4 functional predicts, in just the same way as the FaNDF0 functional, a spherical shape for all nuclei of this region. The remaining three Skyrme EDF versions lead to a deformation of some light lead isotopes, but their number is substantially smaller than that in the case of the HFB-17 and HFB-27 functionals. Moreover, the respective deformation energy is substantially lower, which gives grounds to hope for the restoration of a spherical shape upon going beyond the mean-field approximation, which we use here. Also, the deformation properties of neutron-rich lead isotopes are studied up to the neutron drip line. Here, the results obtained with the FaNDF0 functional are compared with the predictions of the HFB-17, HFB-27, SKM*, and SLy4 Skyrme EDF versions. All of the EDF versions considered here predict the existence of a region where neutron-rich lead isotopes undergo

  15. Oxygen isotope geochemistry of zircon

    NASA Astrophysics Data System (ADS)

    Valley, John W.; Chiarenzelli, Jeffrey R.; McLelland, James M.

    1994-09-01

    The high-temperature and small sample size of an I.R. laser system has allowed the first detailed study of oxygen isotope ratios in zircon. Low-magnetism zircons that have grown during metamorphism in the Adirondack Mts., N.Y. preserve primary delta (O-18) values and low magnetism igneous zircons are likewise primary, showing no significant affect due to subsequent granulite facies metamorphism. The measured fractionation between zircon and garnet is delta (Gt-Zrc) = 0.0 + or - 0.2/mil (1(sigma)) for most low-magnetism zircons in meta-igneous rocks. The consistency of this value indicates equilibration at temperatures of 700 - 1100 C and little or no change in the equilibrium fractionation over this temperature range. In contrast, detrital low-magnetism zircons in quartzite preserve igneous compositions, up to 4/mil out of equilibrium with host quartz, in spite of granulite facies metamorphism. The oxygen isotope composition of zircon can be linked to U-Pb ages and can `see through' metamorphism, providing a new tool for deciphering complex igneous, metamorphic and hydrothermal histories. Zircons separated by magnetic susceptibility show a consistent correlation. Low-magnetism zircons have the lowest uranium contents, the most concordant U-Pb isotopic compositions, and primary delta (O-18) values. In contrast, high-magnetism zircons are up to 2/mil lower in delta (O-18) than low-magnetism zircons from the same rock. The resetting of oxygen isotope ratios in high-magnetism zircons is caused by radiation damage which creates microfractures and enhances isotopic exchange. Zircons from the metamorphosed anorthosite-mangerite-charnocite-granite (AMCG) suite of adirondacks have previously been dated (1125-1157 Ma) and classified as igneous, metamorphic or disturbed based on their physical and U-Pb isotopic characteristics. Low-magnetism zircons from the AMCG suite have high, nearly constant values of delta (O-18) that average 8.1 + or - 0.4/mil(1 sigma) for samples

  16. Modeling equilibrium Fe isotope fractionation

    NASA Astrophysics Data System (ADS)

    Anbar, A.; Jarzecki, A.; Spiro, T.

    2003-04-01

    Research into the stable isotope biogeochemistry of Fe and other transition metals has been driven primarily by analytical innovations which have revealed significant isotope effects in nature and the laboratory. Further development of these new isotope systems requires complementary theoretical research to guide analytical efforts. The results of the first such studies show some discrepancies with experiments. For example, Johnson et al. (2002) report an experimentally-determined 56Fe/54Fe equilibrium fractionation factor between Fe(II) and Fe(III) aquo complexes of ˜1.0025. This effect is ˜50% smaller than predicted theoretically by Schauble et al. (2001). It is important to resolve such discrepancies. Equilibrium isotope fractionation factors can be predicted from vibrational spectroscopic data of isotopically-substituted complexes, or from theoretical predictions of some or all of these frequencies obtained using force field models. The pioneering work of Schauble et al. (2001) utilized a modified Urey-Bradley force field (MUBFF) model. This approach is limiting in at least three ways: First, it is not ab initio, requiring as input some measured vibrational frequencies. Such data are not always available, or may have significant uncertainties. Second, the MUBFF does not include potentially important effects of solvent interaction. Third, because it makes certain assumptions about molecular symmetry, the MUBFF-based approach is not able to model the spectra of mixed-ligand complexes. To address these limitations, we are evaluating the use of density functional theory (DFT) as an ab initio method to predict vibrational frequencies of isotopically-substituted complexes and, hence, equilibrium fractionation factors. In a preliminary examination of the frequency shift upon isotope substitution of the bending and asymmetric stretching modes of the tetrahedral FeCl_42- complex, we find substantial differences between MUBFF and DFT predictions. Results for other Fe

  17. Isotopic anomalies - Chemical memory of Galactic evolution

    NASA Technical Reports Server (NTRS)

    Clayton, Donald D.

    1988-01-01

    New mechanisms for the chemical memory of isotopic anomalies are proposed which are based on the temporal change during the chemical evolution of the Galaxy of the isotopic composition of the mean ejecta from stars. Because of the differing temporal evolution of primary and secondary products of nucleosynthesis, the isotopic composition of the bulk interstellar medium changes approximately linearly with time, and thus any dust component having an age different from that of average dust will be isotopically anomalous. Special attention is given to C, O, Mg, Si, and isotopically heavy average-stellar condensates of SiC.

  18. Isotope hydrology of catchment basins: lithogenic and cosmogenic isotopic systems

    SciTech Connect

    Nimz, G. J., LLNL

    1998-06-01

    A variety of physical processes affect solute concentrations within catchment waters. The isotopic compositions of the solutes can indicate which processes have determined the observed concentrations. These processes together constitute the physical history of the water. Many solutes in natural waters are derived from the interaction between the water and the rock and/or soil within the system - these are termed `lithogenic` solutes. The isotopic compositions of these solutes provide information regarding rock-water interactions. Many other solutes have their isotopic compositions determined both within and outside of the catchment - i.e., in addition to being derived from catchment rock and soil, they are solutes that are also transported into the catchment. Important members of this group include solutes that have isotopic compositions produced by atomic particle interactions with other nuclides. The source of the atomic particles can be cosmic radiation (producing `cosmogenic` nuclides in the atmosphere and land surface), anthropogenic nuclear reactions (producing `thermonuclear` nuclides), or radioactive and fission decay of naturally-occurring elements, principally {sup 238}U (producing `in-situ` lithogenic nuclides in the deep subsurface). Current language usage often combines all of the atomic particle-produced nuclides under the heading `cosmogenic nuclides`, and for simplicity we will often follow that usage here, although always indicating which variety is being discussed. This paper addresses the processes that affect the lithogenic and cosmogenic solute concentrations in catchment waters, and how the isotopic compositions of the solutes can be used in integrative ways to identify these processes, thereby revealing the physical history of the water within a catchment system. The concept of a `system` is important in catchment hydrology. A catchment is the smallest landscape unit that can both participate in all of the aspects of the hydrologic cycle and

  19. Isotopic stack - measurement of heavy cosmic ray isotopes

    NASA Technical Reports Server (NTRS)

    Beaujean, R.

    1981-01-01

    Heavy cosmic ray nuclei with nuclear charge, Z, equal to or greater than 3 are to be measured using an isotopic stack consisting of passive visual track detectors which remain sensitive throughout the entire mission. The scientific data are stored in latent tracks which are produced by heavy ions and which can be revealed in the investigator's laboratory after recovery. During the mission, only housekeeping data have to be collected. The exposure onboard Spacelab 1 allows the study of the chemical composition and energy spectrum of articles which have energies in the range 20 to 100 million electron volts per atomic mass unit, as well as the isotopic composition of heavy galactic cosmic rays with energies in the range 100 to 1000 million electron volts per atomic mass unit.

  20. Developing a Clinically Useful Calcium Isotope Biomarker

    NASA Technical Reports Server (NTRS)

    Romaniello, Stephen J.; Anbar, Ariel D.; Gordon, Gwyneth W.; Skulan, Joseph L.; Smith, Scott M.; Zwart, Sara R.; Monge, Jorge; Fonseca, Rafael

    2016-01-01

    Naturally-occurring Ca is mixture of six isotopes Ca-40, Ca-42, Ca-43, Ca-44, Ca-46, Ca-48). Biological reaction rates and equilibrium constants depend slightly, but measurably, on atomic mass, causing the relative abundances of Ca isotopes to vary between different tissues. During bone formation, light isotopes of Ca are preferentially incorporated into bone, leaving soft tissue depleted in light isotopes. In contrast, bone resorption exhibits no isotopic preference, and thus transfers the light isotope signature of bone back to soft tissue. This balance makes the Ca isotope composition of soft tissue (e.g. serum, urine) a highly sensitive, quantitative tracer for whole-body bone mineral balance (BMB).

  1. Isotopic compositions of the elements, 2001

    USGS Publications Warehouse

    Böhlke, J.K.; De Laeter, J. R.; De Bievre, P.; Hidaka, H.; Peiser, H.S.; Rosman, K.J.R.; Taylor, P.D.P.

    2005-01-01

    The Commission on Atomic Weights and Isotopic Abundances of the International Union of Pure and Applied Chemistry completed its last review of the isotopic compositions of the elements as determined by isotope-ratio mass spectrometry in 2001. That review involved a critical evaluation of the published literature, element by element, and forms the basis of the table of the isotopic compositions of the elements (TICE) presented here. For each element, TICE includes evaluated data from the "best measurement" of the isotope abundances in a single sample, along with a set of representative isotope abundances and uncertainties that accommodate known variations in normal terrestrial materials. The representative isotope abundances and uncertainties generally are consistent with the standard atomic weight of the element A r(E) and its uncertainty U[Ar(E)] recommended by CAWIA in 2001. ?? 2005 American Institute of Physics.

  2. Measuring SNM Isotopic Distributions using FRAM

    SciTech Connect

    Geist, William H.

    2015-12-02

    The first group of slides provides background information on the isotopic composition of plutonium. It is shown that 240Pu is the critical isotope in neutron coincidence/multiplicity counting. Next, response function analysis to determine isotopic composition is discussed. The isotopic composition can be determined by measuring the net peak counts from each isotope and then taking the ratio of the counts for each isotope relative to the total counts for the element. Then FRAM (Fixed energy Response function Analysis with Multiple efficiencies) is explained. FRAM can control data acquisition, automatically analyze newly acquired data, analyze previously acquired data, provide information on the quality of the analysis, and facilitate analysis in unusual situations (non-standard energy calibrations, gamma rays from non-SNM isotopes, poor spectra (within limits)).

  3. Laser ablation molecular isotopic spectrometry of carbon isotopes

    NASA Astrophysics Data System (ADS)

    Bol‧shakov, Alexander A.; Mao, Xianglei; Jain, Jinesh; McIntyre, Dustin L.; Russo, Richard E.

    2015-11-01

    Quantitative determination of carbon isotopes using Laser Ablation Molecular Isotopic Spectrometry (LAMIS) is described. Optical emission of diatomic molecules CN and C2 is used in these measurements. Two quantification approaches are presented: empirical calibration of spectra using a set of reference standards and numerical fitting of a simulated spectrum to the experimental one. Formation mechanisms of C2 and CN in laser ablation plasma are briefly reviewed to provide insights for implementation of LAMIS measurements. A simulated spectrum of the 12C2 Swan system was synthesized using four constituents within 473.5-476.5 nm. Simulation included three branches of 12C2 (1-0), branches R(0-0) and R(1-1), and branch P(9-8) of 12C2. Spectral positions of the tail lines in R(0-0) and R(1-1) were experimentally measured, since they were not accurately known before. The Swan band (1-0) of the isotopologue 13C12C was also simulated. Fitting to the experimental spectrum yielded the ratio 13C/12C = 1.08% in a good agreement with measurements by isotope ratio mass spectrometry. LAMIS promises to be useful in coal, oil and shale exploration, carbon sequestration monitoring, and agronomy studies.

  4. Laser ablation molecular isotopic spectrometry of carbon isotopes

    SciTech Connect

    Bol'shakov, Alexander A.; Jain, Jinesh; Russo, Richard E.; McIntyre, Dustin; Mao, Xianglei

    2015-08-28

    Quantitative determination of carbon isotopes using Laser Ablation Molecular Isotopic Spectrometry (LAMIS) is described. Optical emission of diatomic molecules CN and C2 is used in these measurements. Two quantification approaches are presented:empirical calibration of spectra using a set of reference standards and numerical fitting of a simulated spectrum to the experimental one. Formation mechanisms of C2 and CN in laser ablation plasma are briefly reviewed to provide insights for implementation of LAMIS measurements. A simulated spectrum of the 12C2 Swan system was synthesized using four constituents within 473.5–476.5 nm. Simulation included three branches of 12C2 (1-0), branches R(0-0) and R(1-1), and branch P(9-8) of 12C2. Spectral positions of the tail lines in R(0-0) and R(1-1) were experimentally measured, since they were not accurately known before. The Swan band (1-0) of the isotopologue 13C12C was also simulated. Fitting to the experimental spectrumyielded the ratio 13C/12C = 1.08% in a good agreement with measurements by isotope ratio mass spectrometry. LAMIS promises to be useful in coal, oil and shale exploration, carbon sequestration monitoring, and agronomy studies

  5. Nitrogen isotope effects induced by anammox bacteria

    PubMed Central

    Brunner, Benjamin; Contreras, Sergio; Lehmann, Moritz F.; Matantseva, Olga; Rollog, Mark; Kalvelage, Tim; Klockgether, Gabriele; Lavik, Gaute; Jetten, Mike S. M.; Kartal, Boran; Kuypers, Marcel M. M.

    2013-01-01

    Nitrogen (N) isotope ratios (15N/14N) provide integrative constraints on the N inventory of the modern ocean. Anaerobic ammonium oxidation (anammox), which converts ammonium and nitrite to dinitrogen gas (N2) and nitrate, is an important fixed N sink in marine ecosystems. We studied the so far unknown N isotope effects of anammox in batch culture experiments. Anammox preferentially removes 14N from the ammonium pool with an isotope effect of +23.5‰ to +29.1‰, depending on factors controlling reversibility. The N isotope effects during the conversion of nitrite to N2 and nitrate are (i) inverse kinetic N isotope fractionation associated with the oxidation of nitrite to nitrate (−31.1 ± 3.9‰), (ii) normal kinetic N isotope fractionation during the reduction of nitrite to N2 (+16.0 ± 4.5‰), and (iii) an equilibrium N isotope effect between nitrate and nitrite (−60.5 ± 1.0‰), induced when anammox is exposed to environmental stress, leading to the superposition of N isotope exchange effects upon kinetic N isotope fractionation. Our findings indicate that anammox may be responsible for the unresolved large N isotope offsets between nitrate and nitrite in oceanic oxygen minimum zones. Irrespective of the extent of N isotope exchange between nitrate and nitrite, N removed from the combined nitrite and nitrate (NOx) pool is depleted in 15N relative to NOx. This net N isotope effect by anammox is superimposed on the N isotope fractionation by the co-occurring reduction of nitrate to nitrite in suboxic waters, possibly enhancing the overall N isotope effect for N loss from oxygen minimum zones. PMID:24191043

  6. Isotopic ratios in planetary atmospheres.

    PubMed

    de Bergh, C

    1995-03-01

    Recent progress on measurements of isotopic ratios in planetary or satellite atmospheres include measurements of the D/H ratio in the methane of Uranus, Neptune and Titan and in the water of Mars and Venus. Implications of these measurements on our understanding of the formation and evolution of the planets and satellite are discussed. Our current knowledge of the carbon, nitrogen and oxygen isotopic ratios in the atmospheres of these planets, as well as on Jupiter and Saturn, is also reviewed. We finally show what progress can be expected in the very near future due to some new ground-based instrumentation particularly well suited to such studies, and to forthcoming space missions. PMID:11539257

  7. Interstellar Isotopes: Prospects with ALMA

    NASA Technical Reports Server (NTRS)

    Charnley Steven B.

    2010-01-01

    Cold molecular clouds are natural environments for the enrichment of interstellar molecules in the heavy isotopes of H, C, N and O. Anomalously fractionated isotopic material is found in many primitive Solar System objects, such as meteorites and comets, that may trace interstellar matter that was incorporated into the Solar Nebula without undergoing significant processing. Models of the fractionation chemistry of H, C, N and O in dense molecular clouds, particularly in cores where substantial freeze-out of molecules on to dust has occurred, make several predictions that can be tested in the near future by molecular line observations. The range of fractionation ratios expected in different interstellar molecules will be discussed and the capabilities of ALMA for testing these models (e.g. in observing doubly-substituted isotopologues) will be outlined.

  8. Measuring Oxygen Isotopes with COSIMA

    NASA Astrophysics Data System (ADS)

    Paquette, J. A.; Engrand, C.; Stenzel, O.; Hilchenbach, M.

    2014-12-01

    Oxygen isotopes in a variety of solar system solids show non-mass-dependent fractionation, i.e. are fractionated along a slope = 1 line in a three isotope plot, rather than the equilibrium fractionation line whose slope is close to 0.5 (Clayton, 1973). Many models have been put forward to explain this observation, such as galactic chemical evolution (Clayton, 1988), photochemical self-shielding (Thiemens and Jackson, 1987; Clayton, 2002; Yurimoto and Kuramoto, 2004; Lyons and Young, 2005), quantum chemical explanations (Hathorn and Marcus, 1999, 2000; Gao and Marcus, 2002; Marcus, 2004), the processing of solids via nebular lightning (Nuth et al, 2011), and others. Some of the models were invalidated when the Genesis results showed that the oxygen isotopic fractionation of solar wind (and hence of the Sun) was relatively much richer in 16O than such bodies as the Earth or the Moon. Whatever the process that produced non-mass-dependent fractionation in some chondrules and calcium aluminum inclusions, its signature may also be detectable in other solar system solids. If at least some cometary dust was produced in the inner nebula and only later transported outward to be incorporated into comets, then such dust may also show some degree of non-mass-dependent fractionation. The COSIMA instrument on the Rosetta spacecraft (Kissel et al 2009) is a secondary ion mass spectrometer designed to measure the composition of cometary dust. Using calibration data from the COSIMA reference model and flight data if possible, measurement all three isotopes of oxygen will be attempted, and the results compared to other solar system bodies.

  9. Isotope Labeling in Mammalian Cells

    PubMed Central

    Dutta, Arpana; Saxena, Krishna; Klein-Seetharaman, Judith

    2011-01-01

    Isotope labeling of proteins represents an important and often required tool for the application of nuclear magnetic resonance (NMR) spectroscopy to investigate the structure and dynamics of proteins. Mammalian expression systems have conventionally been considered to be too weak and inefficient for protein expression. However, recent advances have significantly improved the expression levels of these systems. Here, we provide an overview of some of the recent developments in expression strategies for mammalian expression systems in view of NMR investigations. PMID:22167668

  10. Analysis of hydrogen isotope mixtures

    DOEpatents

    Villa-Aleman, Eliel

    1994-01-01

    An apparatus and method for determining the concentrations of hydrogen isotopes in a sample. Hydrogen in the sample is separated from other elements using a filter selectively permeable to hydrogen. Then the hydrogen is condensed onto a cold finger or cryopump. The cold finger is rotated as pulsed laser energy vaporizes a portion of the condensed hydrogen, forming a packet of molecular hydrogen. The desorbed hydrogen is ionized and admitted into a mass spectrometer for analysis.

  11. Rare Isotope Accelerator (RIA) Project

    NASA Astrophysics Data System (ADS)

    York, R. C.

    2006-07-01

    The proposed Rare Isotope Accelerator (RIA) Project will provide world-class intensities of radioactive beams created by any of the known production mechanisms. A driver linac will be used to accelerate any stable isotope from protons through uranium to energies of ⩾400 MeV/u and intensities of ⩾100 kW. Lighter elements will be used to produce radioactive ion beams by the isotope separation on line (ISOL) method. Typically heavier elements will be used to produce radioactive ion beams by the particle fragmentation (PF) method. A hybrid method of stopping radioactive ion beams produced by the PF method in a gas cell will also be employed. The RIA project has strong support from the nuclear science community as evidenced by RIA being the highest priority for major new construction in the most recent Nuclear Science Advisory Committee (NSAC) Long Range Plan [2002 NSAC Long-Range Plan: Opportunities in Nuclear Science, A long-range plan for the next decade, April 2002]. In addition, RIA is tied for third position for the near term priorities of the Department of Energy (DoE) 20-year plan [DOE Office of Science, Facilities for the future of science: a twenty-year outlook. http://www.sc.doe.gov/Sub/Facilities_for_future/facilities_future.htm]. The status of the RIA design is presented.

  12. Large Isotope Spectrometer for Astromag

    NASA Technical Reports Server (NTRS)

    Binns, W. R.; Klarmann, J.; Israel, M. H.; Garrard, T. L.; Mewaldt, R. A.; Stone, E. C.; Ormes, J. F.; Streitmatter, R. E.; Rasmussen, I. L.; Wiedenbeck, M. E.

    1990-01-01

    The Large Isotope Spectrometer for Astromag (LISA) is an experiment designed to measure the isotopic composition and energy spectra of cosmic rays for elements extending from beryllium through zinc. The overall objectives of this investigation are to study the origin and evolution of galactic matter; the acceleration, transport, and time scales of cosmic rays in the galaxy; and search for heavy antinuclei in the cosmic radiation. To achieve these objectives, the LISA experiment will make the first identifications of individual heavy cosmic ray isotopes in the energy range from about 2.5 to 4 GeV/n where relativistic time dilation effects enhance the abundances of radioactive clocks and where the effects of solar modulation and cross-section variations are minimized. It will extend high resolution measurements of individual element abundances and their energy spectra to energies of nearly 1 TeV/n, and has the potential for discovering heavy anti-nuclei which could not have been formed except in extragalactic sources.

  13. Discovery of Cadmium, Indium, and Tin Isotopes

    NASA Astrophysics Data System (ADS)

    Amos, Stephanie; Thoennessen, Michael

    2009-10-01

    As of today, no comprehensive study has been made covering the initial observations and identifications of isotopes. A project has been undertaken at MSU to document the discovery of all the known isotopes. The criteria defining discovery of a given isotope is the publication of clear mass and element assignment in a refereed journal. Prior to the current work the documentation of the discovery of eleven elements had been completed^1. These elements are cerium^2, arsenic, gold, tungsten, krypton, silver, vanadium, einsteinium, iron, barium, and cobalt. We will present the new documentation for the cadmium, indium, and tin isotopes. Thirty-seven cadmium isotopes, thirty-eight indium isotopes, and thirty-eight tin isotopes have been discovered so far. The description for each discovered isotope includes the year of discovery, the article published on the discovery, the article's author, the method of production, the method of identification, and any previous information concerning the isotope discovery. A summary and overview of all ˜500 isotopes documented so far as a function of discovery year, method and place will also be presented. ^1http://www.nscl.msu.edu/˜thoennes/2009/discovery.htm ^2J.Q. Ginepro, J. Snyder, and M. Thoennessen, At. Data Nucl. Data. Tables, in press (2009), doi:10.1016/j.adt.2009.06.002

  14. Unusual mercury isotopic compositions in aqueous environment

    NASA Astrophysics Data System (ADS)

    Chen, J.; Hintelmann, H.; Zheng, W.; Feng, X.; Cai, H.; Wang, Z.; Yuan, S.

    2014-12-01

    Preliminary studies have demonstrated both mass-dependent fractionation (MDF) and mass-independent fractionation (MIF) of Hg isotopes in natural samples. Laboratory experiments showed that photochemical reduction of inorganic mercury (iHg) and methylmercury (MMHg) and liquid-vapour evaporation could produce MIF of odd Hg isotopes. This was thought to cause the MIF actually observed in aquatic organisms. Although isotopic measurements of Hg in aqueous environment would give direct evidence, little data was reported for surface water samples. Recent work reported, unexpectedly, positive MIF of odd Hg isotopes in both precipitation and ambient air, in contrast with the prediction of laboratory experiments and measurements of Hg accumulated in lichens . Intriguingly, MIF of even-mass Hg isotope (200Hg) was also recently determined in the atmosphere. In contrast with the now mainstream observation of odd Hg isotope anomaly that has several theoretical explanations, the hitherto mysterious even Hg isotope anomalies were neither reported in laboratory experiments, nor predicted by isotope fractionation mechanisms, highlighting the importance of further study on Hg isotopes in variable systems. Our measurements of lichens and lake water samples from different countries show for the first time significant Δ200Hg in surface terrestrial reservoirs, realizing a direct connection of even Hg isotope anomaly in the terrestrial reservoirs to the atmospheric deposition, and fulfilling the gap of Δ200Hg between the atmosphere and the terrestrial receptors. The specific odd Hg isotope compositions determined in lake waters also support the atmosphere contribution, and may be directly linked to the high Δ199Hg values largely determined and manifested on the top of aqueous food web. Our data show that the watershed Hg input is another contributing source, rather than the in-lake processes, to explain the lacustrine Hg isotope anomalies. Interestingly, lake sediments are isotopically

  15. A novel methodology to investigate isotopic biosignatures

    NASA Astrophysics Data System (ADS)

    Horner, T. J.; Lee, R. B. Y.; Henderson, G. M.; Rickaby, R. E. M.

    2012-04-01

    An enduring goal of trace metal isotopic studies of Earth History is to find isotopic 'fingerprints' of life or of life's individual physiochemical processes. Generally, such signatures are sought by relating an isotopic effect observed in controlled laboratory conditions or a well-characterized environment to a more complex system or the geological record. However, such an approach is ultimately limited because life exerts numerous isotopic fractionations on any one element so it is hard to dissect the resultant net fractionation into its individual components. Further, different organisms, often with the same apparent cellular function, can express different isotopic fractionation factors. We have used a novel method to investigate the isotopic fractionation associated with a single physiological process-enzyme specific isotopic fractionation. We selected Cd isotopes since only one biological use of Cd is known, CdCA (a Cd/Zn carbonic anhydrase from the coastal diatom T. Weissflogii). Thus, our investigation can also inform the long standing mystery as to why this generally toxic element appears to have a nutrient-like dissolved isotopic and concentration profile in the oceans. We used the pET-15b plasmid to insert the CdCA gene into the E. coli genome. There is no known biochemical function for Cd in E. coli, making it an ideal vector for studying distinct physiological processes within a single organism. The uptake of Cd and associated isotopic fractionation was determined for both normal cells and those expressing CdCA. It was found that whole cells always exhibited a preference for the light isotopes of Cd, regardless of the expression of CdCA; adsorption of Cd to cell surfaces was not seen to cause isotopic fractionation. However, the cleaning procedure employed exerted a strong control on the observed isotopic composition of cells. Using existing protein purification techniques, we measured the Cd isotopic composition of different subcellular fractions of E

  16. Chromium isotopic anomalies in the Murchison meteorite

    NASA Astrophysics Data System (ADS)

    Esat, T. M.; Ireland, T. R.

    1989-02-01

    The abundances of chromium isotopes, in refractory inclusions from the Allende meteorite, show wide-spread anomalies. The chromium isotope anomalies are similar in pattern to the anomalies discovered in Ca and Ti. The largest effects occur at the neutron-rich isotopes Ca-48, Ti-50 and Cr-54. Individual Cr-rich pink spinels, from the Murchison meteorite, exhibit large and variable excesses in Cr-53 and Cr-54 including the largest Cr-53 anomaly so far reported. Magnesium isotopes, in Murchison Cr-poor blue spinels, also show variable anomalies in Mg-26 including mass-dependent fractionation favoring the lighter isotopes. The Cr-53, Cr-54 and Mg-26 anomalies in Murchison spinels are indicative of a heterogeneous distribution of magnesium and chromium isotopes in the early solar nebula and require a contribution from several nucleosynthetic components in addition to physicochemical processing.

  17. Possible isotopic fractionation effects in sputtered minerals

    NASA Technical Reports Server (NTRS)

    Haff, P. K.; Watson, C. C.; Tombrello, T. A.

    1980-01-01

    A model which makes definite predictions for the fractionation of isotopes in sputtered material is discussed. The fractionation patterns are nonlinear, and the pattern for a particular set of isotopes depends on the chemical matrix within which those isotopes are contained. Calculations are presented for all nonmonoisotopic elements contained in the minerals perovskite, anorthite, ackermanite, enstatite, and troilite. All isotopes are fractionated at the level of approximately 4-6 deg/o per atomic mass unit. Oxygen is always positively fractionated (heavier isotopes sputtered preferentially), and heavier elements are generally negatively fractioned (light isotopes sputtered preferentially). The value of Delta (O-18:O-16) is always less by about 1.8 deg/o than a linear extrapolation based upon the calculated delta (O-17:O-16) value would suggest. The phenomenon of both negative and positive fractionation patterns from a single target mineral are used to make an experimental test of the proposed model.

  18. Stable Isotope Signatures for Microbial Forensics

    SciTech Connect

    Kreuzer, Helen W.

    2012-01-03

    The isotopic distribution of the atoms composing the molecules of microorganisms is a function of the substrates used by the organisms. The stable isotope content of an organism is fixed so long as no further substrate consumption and biosynthesis occurs, while the radioactive isotopic content decays over time. The distribution of stable isotopes of C, N, O and H in heterotrophic microorganisms is a direct function of the culture medium, and therefore the stable isotope composition can be used to associate samples with potential culture media and also with one another. The 14C content depends upon the 14C content, and therefore the age, of the organic components of the culture medium, as well as on the age of the culture itself. Stable isotope signatures can thus be used for sample matching, to associate cultures with specific growth media, and to predict characteristics of growth media.

  19. Stable Isotope Enrichment Capabilities at ORNL

    SciTech Connect

    Egle, Brian; Aaron, W Scott; Hart, Kevin J

    2013-01-01

    The Oak Ridge National Laboratory (ORNL) and the US Department of Energy Nuclear Physics Program have built a high-resolution Electromagnetic Isotope Separator (EMIS) as a prototype for reestablishing a US based enrichment capability for stable isotopes. ORNL has over 60 years of experience providing enriched stable isotopes and related technical services to the international accelerator target community, as well as medical, research, industrial, national security, and other communities. ORNL is investigating the combined use of electromagnetic and gas centrifuge isotope separation technologies to provide research quantities (milligram to several kilograms) of enriched stable isotopes. In preparation for implementing a larger scale production facility, a 10 mA high-resolution EMIS prototype has been built and tested. Initial testing of the device has simultaneously collected greater than 98% enriched samples of all the molybdenum isotopes from natural abundance feedstock.

  20. Isotope exchange in oxide-containing catalyst

    NASA Technical Reports Server (NTRS)

    Brown, Kenneth G. (Inventor); Upchurch, Billy T. (Inventor); Hess, Robert V. (Inventor); Miller, Irvin M. (Inventor); Schryer, David R. (Inventor); Sidney, Barry D. (Inventor); Wood, George M. (Inventor); Hoyt, Ronald F. (Inventor)

    1989-01-01

    A method of exchanging rare-isotope oxygen for common-isotope oxygen in the top several layers of an oxide-containing catalyst is disclosed. A sample of an oxide-containing catalyst is exposed to a flowing stream of reducing gas in an inert carrier gas at a temperature suitable for the removal of the reactive common-isotope oxygen atoms from the surface layer or layers of the catalyst without damaging the catalyst structure. The reduction temperature must be higher than any at which the catalyst will subsequently operate. Sufficient reducing gas is used to allow removal of all the reactive common-isotope oxygen atoms in the top several layers of the catalyst. The catalyst is then reoxidized with the desired rare-isotope oxygen in sufficient quantity to replace all of the common-isotope oxygen that was removed.

  1. Absolute isotopic abundances of TI in meteorites

    NASA Astrophysics Data System (ADS)

    Niederer, F. R.; Papanastassiou, D. A.; Wasserburg, G. J.

    1985-03-01

    The absolute isotope abundance of Ti has been determined in Ca-Al-rich inclusions from the Allende and Leoville meteorites and in samples of whole meteorites. The absolute Ti isotope abundances differ by a significant mass dependent isotope fractionation transformation from the previously reported abundances, which were normalized for fractionation using 46Ti/48Ti. Therefore, the absolute compositions define distinct nucleosynthetic components from those previously identified or reflect the existence of significant mass dependent isotope fractionation in nature. The authors provide a general formalism for determining the possible isotope compositions of the exotic Ti from the measured composition, for different values of isotope fractionation in nature and for different mixing ratios of the exotic and normal components.

  2. Quantitative microbial ecology through stable isotope probing.

    PubMed

    Hungate, Bruce A; Mau, Rebecca L; Schwartz, Egbert; Caporaso, J Gregory; Dijkstra, Paul; van Gestel, Natasja; Koch, Benjamin J; Liu, Cindy M; McHugh, Theresa A; Marks, Jane C; Morrissey, Ember M; Price, Lance B

    2015-11-01

    Bacteria grow and transform elements at different rates, and as yet, quantifying this variation in the environment is difficult. Determining isotope enrichment with fine taxonomic resolution after exposure to isotope tracers could help, but there are few suitable techniques. We propose a modification to stable isotope probing (SIP) that enables the isotopic composition of DNA from individual bacterial taxa after exposure to isotope tracers to be determined. In our modification, after isopycnic centrifugation, DNA is collected in multiple density fractions, and each fraction is sequenced separately. Taxon-specific density curves are produced for labeled and nonlabeled treatments, from which the shift in density for each individual taxon in response to isotope labeling is calculated. Expressing each taxon's density shift relative to that taxon's density measured without isotope enrichment accounts for the influence of nucleic acid composition on density and isolates the influence of isotope tracer assimilation. The shift in density translates quantitatively to isotopic enrichment. Because this revision to SIP allows quantitative measurements of isotope enrichment, we propose to call it quantitative stable isotope probing (qSIP). We demonstrated qSIP using soil incubations, in which soil bacteria exhibited strong taxonomic variations in (18)O and (13)C composition after exposure to [(18)O]water or [(13)C]glucose. The addition of glucose increased the assimilation of (18)O into DNA from [(18)O]water. However, the increase in (18)O assimilation was greater than expected based on utilization of glucose-derived carbon alone, because the addition of glucose indirectly stimulated bacteria to utilize other substrates for growth. This example illustrates the benefit of a quantitative approach to stable isotope probing. PMID:26296731

  3. METHOD AND APPARATUS FOR COLLECTING ISOTOPES

    DOEpatents

    Leyshon, W.E.

    1957-08-01

    A method and apparatus for collecting isotopes having a high vapor pressure, such as isotopes of mercury, in a calutron are described. Heretofore, the collected material would vaporize and escape from the ion receiver as fast as it was received. By making the receiver of pure silver, the mercury isotopes form a nonvolatile amalgam with the silver at the water cooled temperature of the receiver, and the mercury is thus retained.

  4. Method for isotope separation by photodeflection

    DOEpatents

    Bernhardt, Anthony F.

    1977-01-01

    In the method of separating isotopes wherein a desired isotope species is selectively deflected out of a beam of mixed isotopes by irradiating the beam with a directed beam of light of narrowly defined frequency which is selectively absorbed by the desired species, the improvement comprising irradiating the deflected beam with light from other light sources whose frequencies are selected to cause the depopulation of any metastable excited states.

  5. Theory of the Helium Isotope Shift

    NASA Astrophysics Data System (ADS)

    Pachucki, Krzysztof; Yerokhin, V. A.

    2015-09-01

    Theory of the isotope shift of the centroid energies of light few-electron atoms is reviewed. Numerical results are presented for the isotope shift of the 23P-23S and 21S-23S transition energies of 3He and 4He. By comparing theoretical predictions for the isotope shift with the experimental results, the difference of the squares of the nuclear charge radii of 3He and 4He, δR2, is determined with high accuracy.

  6. Normalization of oxygen and hydrogen isotope data

    USGS Publications Warehouse

    Coplen, T.B.

    1988-01-01

    To resolve confusion due to expression of isotopic data from different laboratories on non-corresponding scales, oxygen isotope analyses of all substances can be expressed relative to VSMOW or VPDB (Vienna Peedee belemnite) on scales normalized such that the ??18O of SLAP is -55.5% relative to VSMOW. H3+ contribution in hydrogen isotope ratio analysis can be easily determined using two gaseous reference samples that differ greatly in deuterium content. ?? 1988.

  7. Multiple linear regression for isotopic measurements

    NASA Astrophysics Data System (ADS)

    Garcia Alonso, J. I.

    2012-04-01

    There are two typical applications of isotopic measurements: the detection of natural variations in isotopic systems and the detection man-made variations using enriched isotopes as indicators. For both type of measurements accurate and precise isotope ratio measurements are required. For the so-called non-traditional stable isotopes, multicollector ICP-MS instruments are usually applied. In many cases, chemical separation procedures are required before accurate isotope measurements can be performed. The off-line separation of Rb and Sr or Nd and Sm is the classical procedure employed to eliminate isobaric interferences before multicollector ICP-MS measurement of Sr and Nd isotope ratios. Also, this procedure allows matrix separation for precise and accurate Sr and Nd isotope ratios to be obtained. In our laboratory we have evaluated the separation of Rb-Sr and Nd-Sm isobars by liquid chromatography and on-line multicollector ICP-MS detection. The combination of this chromatographic procedure with multiple linear regression of the raw chromatographic data resulted in Sr and Nd isotope ratios with precisions and accuracies typical of off-line sample preparation procedures. On the other hand, methods for the labelling of individual organisms (such as a given plant, fish or animal) are required for population studies. We have developed a dual isotope labelling procedure which can be unique for a given individual, can be inherited in living organisms and it is stable. The detection of the isotopic signature is based also on multiple linear regression. The labelling of fish and its detection in otoliths by Laser Ablation ICP-MS will be discussed using trout and salmon as examples. As a conclusion, isotope measurement procedures based on multiple linear regression can be a viable alternative in multicollector ICP-MS measurements.

  8. THEORETICAL AND EXPERIMENTAL ASPECTS OF ISOTOPIC FRACTIONATION.

    USGS Publications Warehouse

    O'Neil, James R.

    1986-01-01

    Essential to the interpretation of natural variations of light stable isotope ratios is knowledge of the magnitude and temperature dependence of isotopic fractionation factors between the common minerals and fluids. These fractionation factors are obtained in three ways: (1) Semi-empirical calculations using spectroscopic data and the methods of statistical mechanics. (2) Laboratory calibration studies. (3) Measurements of natural samples whose formation conditions are well-known or highly constrained. In this chapter methods (1) and (2) are evaluated and a review is given of the present state of knowledge of the theory of isotopic fractionation and the fraction that influence the isotopic properties of minerals.

  9. Atom trap trace analysis of krypton isotopes

    SciTech Connect

    Bailey, K.; Chen, C. Y.; Du, X.; Li, Y. M.; Lu, Z.-T.; O'Connor, T. P.; Young, L.

    1999-11-17

    A new method of ultrasensitive isotope trace analysis has been developed. This method, based on the technique of laser manipulation of neutral atoms, has been used to count individual {sup 85}Kr and {sup 81}Kr atoms present in a natural krypton gas sample with isotopic abundances in the range of 10{sup {minus}11} and 10{sup {minus}13}, respectively. This method is free of contamination from other isotopes and elements and can be applied to several different isotope tracers for a wide range of applications. The demonstrated detection efficiency is 1 x 10{sup {minus}7}. System improvements could increase the efficiency by many orders of magnitude.

  10. Variable Carbon Isotopes in ALH84001 Carbonates

    NASA Astrophysics Data System (ADS)

    Niles, P. B.; Leshin, L. A.; Guan, Y.

    2002-12-01

    The Martian meteorite ALH84001 contains a small amount of carbonate that was deposited from aqueous fluids on the Martian surface approximately 3.9 Ga.. McKay et al. (1996) proposed evidence for the existence of life preserved within the carbonate grains. In order to determine the nature of the ancient Martian aqueous system we have combined previously collected oxygen isotopic data with new carbon isotopic measurements performed on the Cameca 6f ion microprobe at Arizona State University. Isotopic measurements were made at high mass resolution with a spot size of 10 microns. The measured carbon isotopic values range from 29.2‰ to 64.5‰ (PDB) with an average uncertainty of +/-1.6‰ (1σ ). These data agree very well with previous acid dissolution and stepped combustion experiments which range from a δ13C of +32‰ to +41‰ . As observed with the oxygen isotopic data, the carbon isotopic composition is correlated with the chemical composition of the carbonates. This allows us to establish that the earliest (Ca-rich) carbonates had the lightest carbon isotopic composition while the latest forming (Mg-rich) carbonates had the heaviest carbon isotopic composition. The large range of carbon isotopic compositions measured in this study cannot be explained by previously proposed models. Temperature change or a Rayleigh distillation process caused by progressive carbonate precipitation are insufficient to create the observed carbon isotopic compositions. Furthermore, processes such as evaporation or photosynthesis will not produce large carbon isotopic variations due to rapid isotopic equilibration with the atmosphere. We propose two possible models for the formation of the ALH84001 carbonates consistent with the isotopic data collected thus far. Carbonates could have formed from an evolving system where the carbon and oxygen isotopic composition of the carbonates reflects a mixing between magmatic hydrothermal fluids and fluids in equilibrium with an isotopically

  11. Carbon isotopic composition of Amazon shelf sediments

    SciTech Connect

    Showers, W.J.; Angle, D.G.; Nittrouer, C.A.; Demaster, D.J.

    1985-02-01

    The distribution of carbon isotopes in Amazon shelf sediment is controlled by the same processes that are forming the modern subaqueous delta. The terrestrial (-27 to -25 per thousand) isotopic carbon signal observed in surficial sediments near the river mouth extends over 400 km northwest along the shelf. Terrestrial carbon is associated with areas of rapid sediment accumulation (topset and foreset regions). A sharp boundary between terrestrial (-27 to -25 per thousand) and marine (-23 to -22 per thousand) isotopic carbon values in surficial sediments is associated with a change in depositional conditions (foreset to bottomset regions) and a decrease in sediment accumulation rate. POC water-column isotopic values (-27 per thousand) near the river mouth are similar to the underlying surficial-sediment TOC isotopic values, but POC water-column samples collected 20 km off the river mouth have marine carbon isotopic values (-22 to -19 per thousand) and differ from the underlying surficial-sediment TOC isotopic values. These water column observations are related to variations in turbidity and productivity. Down-core isotopic variation is only observed in cores taken in areas of lower sediment accumulation rates. These observations indicate that the organic carbon in Amazon shelf sediment is dominantly terrestrial in composition, and the location of deposition of this carbon is controlled by modern processes of sediment accumulation. The modern Amazon shelf is similar to large clinoform shale deposits of the Cretaceous in North America. Thus, the stratigraphic setting may help predict the isotopic variations of carbon in ancient deposits.

  12. Method for isotope enrichment by photoinduced chemiionization

    DOEpatents

    Dubrin, James W.

    1985-01-01

    Isotope enrichment, particularly .sup.235 U enrichment, is achieved by irradiating an isotopically mixed vapor feed with radiant energy at a wavelength or wavelengths chosen to selectively excite the species containing a desired isotope to a predetermined energy level. The vapor feed if simultaneously reacted with an atomic or molecular reactant species capable of preferentially transforming the excited species into an ionic product by a chemiionization reaction. The ionic product, enriched in the desired isotope, is electrostatically or electromagnetically extracted from the reaction system.

  13. Adsorption and isotopic fractionation of Xe

    NASA Technical Reports Server (NTRS)

    Bernatowicz, T. J.; Podosek, F. A.

    1986-01-01

    A theoretical description of the mechanisms of isotopic fractionation arising during adsorption of noble gases in a Henry's Law pressure regime is given. Experimental data on the isotopic composition of Xe adsorbed on activated charcoal in the temperature range 220 K to 350 K are presented. Both theoretical considerations and the experimental data indicate that equilibrium adsorption does not significantly alter the isotopic structure of adsorbed structure of adsorbed noble gases. Therefore, if adsorption is responsible for the elemental noble gas pattern in meteorites and the earth, the heavy noble gas isotopic fractionation between them must have been produced prior to and by a different process than equilibrium adsorption.

  14. Miniature Laser Spectrometer for Stable Isotope Measurements

    NASA Technical Reports Server (NTRS)

    Becker, J. F.; Kojiro, D. R.

    1999-01-01

    As a first step in successfully measuring carbon isotopes optically we have previously demonstrated the measurement of C-13/C-12 to a precision of 0.1% using a tunable diode laser and CO2 spectral lines in the 2300/cm spectral region. This precision of 0.1% (1 per mil) for carbon isotopes is a value sufficiently precise to provide important isotopic data of interest to astrobiologists. The precision presently attainable in gases is sufficient to permit our instrument to be used in the measurement of isotopic ratios of interest to astrobiologists as well as geologists and planetary scientists.

  15. Stable isotope labeling methods for DNA.

    PubMed

    Nelissen, Frank H T; Tessari, Marco; Wijmenga, Sybren S; Heus, Hans A

    2016-08-01

    NMR is a powerful method for studying proteins and nucleic acids in solution. The study of nucleic acids by NMR is far more challenging than for proteins, which is mainly due to the limited number of building blocks and unfavorable spectral properties. For NMR studies of DNA molecules, (site specific) isotope enrichment is required to facilitate specific NMR experiments and applications. Here, we provide a comprehensive review of isotope-labeling strategies for obtaining stable isotope labeled DNA as well as specifically stable isotope labeled building blocks required for enzymatic DNA synthesis. PMID:27573183

  16. Isotopic characteristics of Indian precipitation

    NASA Astrophysics Data System (ADS)

    Kumar, Bhishm; Rai, S. P.; Kumar, U. Saravana; Verma, S. K.; Garg, Pankaj; Kumar, S. V. Vijaya; Jaiswal, Rahul; Purendra, B. K.; Kumar, S. R.; Pande, N. G.

    2010-12-01

    Hydrogen (2H/1H) and oxygen (18O/16O) isotopic ratios were measured in precipitation (900 samples) collected from several locations in India during the period 2003-2006 (12 locations in 2003 and 18 locations in 2004-2006). The amount of rainfall along with air temperature and humidity were also measured. The meteoric water line developed for India using isotopic data of precipitation samples, namely, δ2H = 7.93(±0.06) × δ18O + 9.94(±0.51) (n = 272, r2 = 0.98), differs slightly from the global meteoric water line. Regional meteoric water lines were developed for several Indian regions (i.e., northern and southern regions of India, western Himalayas) and found to be different from each other (southern Indian meteoric water line, slope is 7.82, intercept or D excess is 10.23; northern Indian meteoric water line, slope is 8.15, intercept is 9.55) which is attributed to differences in their geographic and meteorological conditions and their associated atmospheric processes (i.e., ambient temperature, humidity, organ, and source of vapor masses). The local meteoric water lines developed for a number of locations show wide variations in the slope and intercept. These variations are due to different vapor sources such as the northeast (NE) monsoon that originates in the Bay of Bengal; the southwest monsoon (SW) that originates in the Arabian Sea; a mixture of NE and SW monsoons; retreat of NE and SW monsoons and western disturbances that originate in the Mediterranean Sea. The altitude effect in the isotopic composition of precipitation estimated for western Himalayan region also varies from month to month.

  17. Uranium isotopes fingerprint biotic reduction

    SciTech Connect

    Stylo, Malgorzata; Neubert, Nadja; Wang, Yuheng; Monga, Nikhil; Romaniello, Stephen J.; Weyer, Stefan; Bernier-Latmani, Rizlan

    2015-04-20

    Knowledge of paleo-redox conditions in the Earth’s history provides a window into events that shaped the evolution of life on our planet. The role of microbial activity in paleo-redox processes remains unexplored due to the inability to discriminate biotic from abiotic redox transformations in the rock record. The ability to deconvolute these two processes would provide a means to identify environmental niches in which microbial activity was prevalent at a specific time in paleo-history and to correlate specific biogeochemical events with the corresponding microbial metabolism. Here, we demonstrate that the isotopic signature associated with microbial reduction of hexavalent uranium (U), i.e., the accumulation of the heavy isotope in the U(IV) phase, is readily distinguishable from that generated by abiotic uranium reduction in laboratory experiments. Thus, isotope signatures preserved in the geologic record through the reductive precipitation of uranium may provide the sought-after tool to probe for biotic processes. Because uranium is a common element in the Earth’s crust and a wide variety of metabolic groups of microorganisms catalyze the biological reduction of U(VI), this tool is applicable to a multiplicity of geological epochs and terrestrial environments. The findings of this study indicate that biological activity contributed to the formation of many authigenic U deposits, including sandstone U deposits of various ages, as well as modern, Cretaceous, and Archean black shales. In addition, engineered bioremediation activities also exhibit a biotic signature, suggesting that, although multiple pathways may be involved in the reduction, direct enzymatic reduction contributes substantially to the immobilization of uranium.

  18. Uranium isotopes fingerprint biotic reduction

    DOE PAGESBeta

    Stylo, Malgorzata; Neubert, Nadja; Wang, Yuheng; Monga, Nikhil; Romaniello, Stephen J.; Weyer, Stefan; Bernier-Latmani, Rizlan

    2015-04-20

    Knowledge of paleo-redox conditions in the Earth’s history provides a window into events that shaped the evolution of life on our planet. The role of microbial activity in paleo-redox processes remains unexplored due to the inability to discriminate biotic from abiotic redox transformations in the rock record. The ability to deconvolute these two processes would provide a means to identify environmental niches in which microbial activity was prevalent at a specific time in paleo-history and to correlate specific biogeochemical events with the corresponding microbial metabolism. Here, we demonstrate that the isotopic signature associated with microbial reduction of hexavalent uranium (U),more » i.e., the accumulation of the heavy isotope in the U(IV) phase, is readily distinguishable from that generated by abiotic uranium reduction in laboratory experiments. Thus, isotope signatures preserved in the geologic record through the reductive precipitation of uranium may provide the sought-after tool to probe for biotic processes. Because uranium is a common element in the Earth’s crust and a wide variety of metabolic groups of microorganisms catalyze the biological reduction of U(VI), this tool is applicable to a multiplicity of geological epochs and terrestrial environments. The findings of this study indicate that biological activity contributed to the formation of many authigenic U deposits, including sandstone U deposits of various ages, as well as modern, Cretaceous, and Archean black shales. In addition, engineered bioremediation activities also exhibit a biotic signature, suggesting that, although multiple pathways may be involved in the reduction, direct enzymatic reduction contributes substantially to the immobilization of uranium.« less

  19. Uranium isotopes fingerprint biotic reduction.

    PubMed

    Stylo, Malgorzata; Neubert, Nadja; Wang, Yuheng; Monga, Nikhil; Romaniello, Stephen J; Weyer, Stefan; Bernier-Latmani, Rizlan

    2015-05-01

    Knowledge of paleo-redox conditions in the Earth's history provides a window into events that shaped the evolution of life on our planet. The role of microbial activity in paleo-redox processes remains unexplored due to the inability to discriminate biotic from abiotic redox transformations in the rock record. The ability to deconvolute these two processes would provide a means to identify environmental niches in which microbial activity was prevalent at a specific time in paleo-history and to correlate specific biogeochemical events with the corresponding microbial metabolism. Here, we demonstrate that the isotopic signature associated with microbial reduction of hexavalent uranium (U), i.e., the accumulation of the heavy isotope in the U(IV) phase, is readily distinguishable from that generated by abiotic uranium reduction in laboratory experiments. Thus, isotope signatures preserved in the geologic record through the reductive precipitation of uranium may provide the sought-after tool to probe for biotic processes. Because uranium is a common element in the Earth's crust and a wide variety of metabolic groups of microorganisms catalyze the biological reduction of U(VI), this tool is applicable to a multiplicity of geological epochs and terrestrial environments. The findings of this study indicate that biological activity contributed to the formation of many authigenic U deposits, including sandstone U deposits of various ages, as well as modern, Cretaceous, and Archean black shales. Additionally, engineered bioremediation activities also exhibit a biotic signature, suggesting that, although multiple pathways may be involved in the reduction, direct enzymatic reduction contributes substantially to the immobilization of uranium. PMID:25902522

  20. Uranium isotopes fingerprint biotic reduction

    PubMed Central

    Stylo, Malgorzata; Neubert, Nadja; Wang, Yuheng; Monga, Nikhil; Romaniello, Stephen J.; Weyer, Stefan; Bernier-Latmani, Rizlan

    2015-01-01

    Knowledge of paleo-redox conditions in the Earth’s history provides a window into events that shaped the evolution of life on our planet. The role of microbial activity in paleo-redox processes remains unexplored due to the inability to discriminate biotic from abiotic redox transformations in the rock record. The ability to deconvolute these two processes would provide a means to identify environmental niches in which microbial activity was prevalent at a specific time in paleo-history and to correlate specific biogeochemical events with the corresponding microbial metabolism. Here, we demonstrate that the isotopic signature associated with microbial reduction of hexavalent uranium (U), i.e., the accumulation of the heavy isotope in the U(IV) phase, is readily distinguishable from that generated by abiotic uranium reduction in laboratory experiments. Thus, isotope signatures preserved in the geologic record through the reductive precipitation of uranium may provide the sought-after tool to probe for biotic processes. Because uranium is a common element in the Earth’s crust and a wide variety of metabolic groups of microorganisms catalyze the biological reduction of U(VI), this tool is applicable to a multiplicity of geological epochs and terrestrial environments. The findings of this study indicate that biological activity contributed to the formation of many authigenic U deposits, including sandstone U deposits of various ages, as well as modern, Cretaceous, and Archean black shales. Additionally, engineered bioremediation activities also exhibit a biotic signature, suggesting that, although multiple pathways may be involved in the reduction, direct enzymatic reduction contributes substantially to the immobilization of uranium. PMID:25902522

  1. Spatial periphery of lithium isotopes

    SciTech Connect

    Galanina, L. I. Zelenskaja, N. S.

    2013-12-15

    The spatial structure of lithium isotopes is studied with the aid of the charge-exchange and (t, p) reactions on lithium nuclei. It is shown that an excited isobaric-analog state of {sup 6}Li (0{sup +}, 3.56MeV) has a halo structure formed by a proton and a neutron, that, in the {sup 9}Li nucleus, there is virtually no neutron halo, and that {sup 11}Li is a Borromean nucleus formed by a {sup 9}Li core and a two-neutron halo manifesting itself in cigar-like and dineutron configurations.

  2. Hydrogen-isotope permeation barrier

    DOEpatents

    Maroni, Victor A.; Van Deventer, Erven H.

    1977-01-01

    A composite including a plurality of metal layers has a Cu-Al-Fe bronze layer and at least one outer layer of a heat and corrosion resistant metal alloy. The bronze layer is ordinarily intermediate two outer layers of metal such as austenitic stainless steel, nickel alloys or alloys of the refractory metals. The composite provides a barrier to hydrogen isotopes, particularly tritium that can reduce permeation by at least about 30 fold and possibly more below permeation through equal thicknesses of the outer layer material.

  3. Selectivity of bis-triazinyl bipyridine ligands for americium(III) in Am/Eu separation by solvent extraction. Part 1. Quantum mechanical study on the structures of BTBP complexes and on the energy of the separation.

    PubMed

    Narbutt, Jerzy; Oziminski, Wojciech P

    2012-12-21

    Theoretical studies were carried out on two pairs of americium and europium complexes formed by tetra-N-dentate lipophilic BTBP ligands, neutral [ML(NO(3))(3)] and cationic [ML(2)](3+) where M = Am(III) or Eu(III), and L = 6,6'-bis-(5,6-diethyl-1,2,4-triazin-3-yl)-2,2'-bipyridine (C2-BTBP). Molecular structures of the complexes have been optimized at the B3LYP/6-31G(d) level and total energies of the complexes in various media were estimated using single point calculations performed at the B3LYP/6-311G(d,p) and MP2/6-311G(d,p) levels of theory. In the calculations americium and europium ions were treated using pseudo-relativistic Stuttgart-Dresden effective core potentials and the accompanying basis sets. Selectivity in solvent extraction separation of two metal ions is a co-operative function of contributions from all extractable metal complexes, which depend on physico-chemical properties of each individual complex and on its relative amount in the system. Semi-quantitative analysis of BTBP selectivity in the Am/Eu separation process, based on the contributions from the two pairs of Am(III) and Eu(III) complexes, has been carried out. To calculate the energy of Am/Eu separation, a model of the extraction process was used, consisting of complex formation in water and transfer of the formed complex to the organic phase. Under the assumptions discussed in the paper, this simple two-step model results in reliable values of the calculated differences in the energy changes for each pair of the Am/Eu complexes in both steps of the process. The greater thermodynamic stability (in water) of the Am-BTBP complexes, as compared with the analogous Eu species, caused by greater covalency of the Am-N than Eu-N bonds, is most likely the main reason for BTBP selectivity in the separation of the two metal ions. The other potential reason, i.e. differences in lipophilic properties of the analogous complexes of Am and Eu, is less important with regard to this selectivity. PMID

  4. Lithium and magnesium isotopes fractionation by zone melting

    NASA Astrophysics Data System (ADS)

    Akimov, D. V.; Egorov, N. B.; Dyachenko, A. N.; Pustovalova, M. P.; Podoinikov, I. R.

    2016-06-01

    The process of changing isotopic composition of the lithium and magnesium salts was studied by using the process of zone melting. It was founded in the paper that the process of separation of the lithium isotopes is more effective than for magnesium isotopes when the conditions of process were the same. The coefficients of isotopes separation were calculated and have the next value: α = 1.006 for 26Mg isotope and α = 1.0022 for 6Li isotope.

  5. Oxygen isotope geospeedometry by SIMS

    NASA Astrophysics Data System (ADS)

    Bonamici, C. E.; Valley, J. W.

    2013-12-01

    Geospeedometry, a discipline closely related and complimentary to thermochronology, exploits the phenomenon of diffusion in order to extract rate and duration information for segments of a rock's thermal history. Geospeedometry data, when anchored in absolute time by geochronologic data, allow for the construction of detailed temperature-time paths for specific terranes and geologic processes. We highlight the developing field of SIMS-based oxygen isotope geospeedometry with an application from granulites of the Adirondack Mountains (New York) and discuss potential future applications based on a recently updated and expanded modeling tool, the Fast Grain Boundary diffusion program (FGB; Eiler et al. 1994). Equilibrium oxygen isotope ratios in minerals are a function of temperature and bulk rock composition. In dynamic systems, intragrain oxygen isotope zoning can develop in response to geologic events that affect the thermal state of a rock and/or induce recrystallization, especially tectonic deformation and fluid infiltration. As an example, titanite grains from late-Grenville shear zones in the northwestern Adirondack Mountains exhibit a range of δ18O zoning patterns that record post-peak metamorphic cooling, episodic fluid infiltration, and deformation-facilitated recrystallization. Many titanite grains preserve smooth, core-to-rim decreasing, diffusional δ18O profiles, which are amenable to diffusion modeling. FGB models that best fit the measured δ18O profiles indicate cooling from ~700-500°C in just 2-5 m.y., a rapid thermal change signaling the final gravitational collapse of the late-Grenville orogen. Titanite can also be utilized as a U-Pb chronometer, and comparison of δ18O and U-Pb age zoning patterns within the Adirondack titanites pins the episode of rapid cooling inferred from the δ18O record to some time between 1054 and 1047 Ma. The expanded capabilities of FGB also allow for evaluation of a range of heating-cooling histories for the

  6. Advanced Mass Spectrometers for Hydrogen Isotope Analyses

    SciTech Connect

    Chastagner, P.

    2001-08-01

    This report is a summary of the results of a joint Savannah River Laboratory (SRL) - Savannah River Plant (SRP) ''Hydrogen Isotope Mass Spectrometer Evaluation Program''. The program was undertaken to evaluate two prototype hydrogen isotope mass spectrometers and obtain sufficient data to permit SRP personnel to specify the mass spectrometers to replace obsolete instruments.

  7. Iron Isotopic Diagnostics of Presolar Supernova Grains

    NASA Technical Reports Server (NTRS)

    Clayton, D. D.; Meyer, B. S; The, L.-S.

    2002-01-01

    We study the abundance and isotopic composition of iron in a massive-star supernova to identify those isotopic characteristics that can identify the location of the condensing matter that is contained in the presolar supernova grains from meteorites. Additional information is contained in the original extended abstract.

  8. Xenon Isotope Releases from Buried Transuranic Waste

    NASA Astrophysics Data System (ADS)

    Dresel, P. E.; Waichler, S. R.; Kennedy, B. M.; Hayes, J. C.; McIntyre, J. I.; Giles, J. R.; Sondrup, A. J.

    2004-12-01

    Xenon is an inert rare gas produced as a fission product in nuclear reactors and through spontaneous fission of some transuranic isotopes. Thus, xenon will be released from buried transuranic waste. Two complementary methods are used to measure xenon isotopes: radiometric analysis for short-lived radioxenon isotopes and mass spectrometry for detection of stable xenon isotopes. Initial measurements near disposal facilities at the U.S. Department of Energy's Hanford Site show radioxenon and stable xenon isotopic signatures that are indicative of transuranic waste. Radioxenon analysis has greater sensitivity due to the lower background concentrations and indicates spontaneous fission due to the short half life of the isotopes. Stable isotope ratios may be used to distinguish irradiated fuel sources from pure spontaneous fission sources and are not as dependent on rapid release from the waste form. The release rate is dependent on the type of waste and container integrity and is the greatest unknown in application of this technique. Numerical multi-phase transport modeling of burial grounds at the Idaho National Engineering and Environmental Laboratory indicates that, under generalized conditions, the radioxenon isotopes will diffuse away from the waste and be found in the soil cap and adjacent to the burial ground at levels many orders of magnitude above the detection limit.

  9. Isotope separation by selective photodissociation of glyoxal

    DOEpatents

    Marling, John B.

    1976-01-01

    Dissociation products, mainly formaldehyde and carbon monoxide, enriched in a desired isotope of carbon, oxygen, or hydrogen are obtained by the selective photodissociation of glyoxal wherein glyoxal is subjected to electromagnetic radiation of a predetermined wavelength such that photon absorption excites and induces dissociation of only those molecules of glyoxal containing the desired isotope.

  10. [Carbon isotope fractionation inplants]. Final report

    SciTech Connect

    O`Leary, M.H.

    1990-12-31

    The objectives of this research are: To develop a theoretical and experimental framework for understanding isotope fractionations in plants; and to develop methods for using this isotope fractionation for understanding the dynamics of CO{sub 2} fixation in plants. Progress is described.

  11. Isotope effect of mercury diffusion in air

    PubMed Central

    Koster van Groos, Paul G.; Esser, Bradley K.; Williams, Ross W.; Hunt, James R.

    2014-01-01

    Identifying and reducing impacts from mercury sources in the environment remains a considerable challenge and requires process based models to quantify mercury stocks and flows. The stable isotope composition of mercury in environmental samples can help address this challenge by serving as a tracer of specific sources and processes. Mercury isotope variations are small and result only from isotope fractionation during transport, equilibrium, and transformation processes. Because these processes occur in both industrial and environmental settings, knowledge of their associated isotope effects is required to interpret mercury isotope data. To improve the mechanistic modeling of mercury isotope effects during gas phase diffusion, an experimental program tested the applicability of kinetic gas theory. Gas-phase elemental mercury diffusion through small bore needles from finite sources demonstrated mass dependent diffusivities leading to isotope fractionation described by a Rayleigh distillation model. The measured relative atomic diffusivities among mercury isotopes in air are large and in agreement with kinetic gas theory. Mercury diffusion in air offers a reasonable explanation of recent field results reported in the literature. PMID:24364380

  12. Amino acid isotopic analysis in agricultural systems

    Technology Transfer Automated Retrieval System (TEKTRAN)

    A relatively new approach to stable isotopic analysis—referred to as compound-specific isotopic analysis (CSIA)—has emerged, centering on the measurement of 15N:14N ratios in amino acids (glutamic acid and phenylalanine). CSIA has recently been used to generate trophic position estimates among anima...

  13. Uses of stable isotopes in fish ecology

    EPA Science Inventory

    Analyses of fish tissues (other than otoliths) for stable isotope ratios can provide substantial information on fish ecology, including physiological ecology. Stable isotopes of nitrogen and carbon frequently are used to determine the mix of diet sources for consumers. Stable i...

  14. Isotopic fractionation of cadmium into calcite

    NASA Astrophysics Data System (ADS)

    Horner, Tristan J.; Rickaby, Rosalind E. M.; Henderson, Gideon M.

    2011-12-01

    Cadmium mimics the distribution of the macronutrient phosphate in the oceans, and has uses as a palaeoproxy of past ocean circulation and nutrient utilization. Isotopic analyses of dissolved Cd in modern seawater show potential as a new tool for disentangling phytoplankton utilization of Cd from abiotic processes, such as ocean mixing. Extending this information into the past requires the Cd isotope signal to be captured and faithfully preserved in a suitable sedimentary archive. However, the role that environmental factors, such as temperature, may play in controlling Cd isotope fractionation into such archives has not been assessed. To this end, we have performed controlled inorganic CaCO 3 precipitation experiments in artificial seawater solutions. We grew calcite under different precipitation rates, temperatures, salinities, and ambient [Mg 2 + ], before measuring Cd isotopic compositions by double spike MC-ICPMS. We find that the isotopic fractionation factor for Cd into calcite ( α-C) in seawater is always less than one (i.e. light isotopes of Cd are preferred in calcite). The fractionation factor has a value of 0.99955 ± 0.00012 and shows no response to temperature, [Mg 2 + ], or precipitation rate across the range studied. The constancy of this fractionation in seawater suggests that marine calcites may provide a record of the local seawater composition, without the need to correct for effects due to environmental variables. We also performed CaCO 3 growth in freshwater and, in contrast to calcite precipitated from artificial seawater solutions, no isotopic offset was recorded between the growth solution and calcite ( α-Cd=1.0000±0.0001). Cadmium isotope fractionation during calcite growth can be explained by a kinetic isotope effect during the largely unidirectional incorporation of Cd at the mineral surface. Further, the rate of Cd uptake and isotopic fractionation can be modulated by increased ion blocking of crystal surface sites at high salinity

  15. Uncertainty induced by chest wall thickness assessment methods on lung activity estimation for plutonium and americium: a large population-based study.

    PubMed

    Broggio, D; Lechaftois, X; Franck, D

    2015-03-01

    In vivo lung counting aims at assessing the retained activity in the lungs. The calibration factor relating the measured counts to the worker's specific retained lung activity can be obtained by several means and strongly depends on the chest wall thickness. Here we compare, for 374 male nuclear workers, the activity assessed with a reference protocol, where the material equivalent chest wall thickness is known from ultrasound measurements, with two other protocols. The counting system is an array of four germanium detectors.It is found that non site-specific equations for the assessment of the chest wall thickness induce large biases in the assessment of activity. For plutonium isotopes or (241)Am the proportion of workers for whom the retained activity is within ± 10% of the reference one is smaller than 10%.The use of site-specific equations raises this proportion to 20% and 58% for plutonium and (241)Am, respectively.Finally, for the studied population, when site-specific equations are used for the chest wall thickness, the standard uncertainties for the lung activity are 42% and 12.5%, for plutonium and (241)Am, respectively. Due to the relatively large size of the studied population, these values are a relatively robust estimate of the uncertainties due to the assessment of the chest wall thickness for the current practice at this site. PMID:25517347

  16. Oxygen isotope fractionation in stratospheric CO2

    NASA Technical Reports Server (NTRS)

    Thiemens, M. H.; Jackson, T.; Mauersberger, K.; Schueler, B.; Morton, J.

    1991-01-01

    A new cryogenic collection system has been flown on board a balloon gondola to obtain separate samples of ozone and carbon dioxide without entrapping major atmospheric gases. Precision laboratory isotopic analysis of CO2 samples collected between 26 and 35.5 km show a mass-independent enrichment in both O-17 and O-18 of about 11 per mil above tropospheric values. Ozone enrichment in its heavy isotopes was 9 to 16 percent in O3-50 and 8 to 11 percent in O3-49, respectively (Schueler et al., 1990). A mechanism to explain the isotope enrichment in CO2 has been recently proposed by Yung et al. (1991). The model is based on the isotope exchange between CO2 and O3 via O(1D), resulting in a transfer of the ozone isotope enrichment to carbon dioxide. Predicted enrichment and measured values agree well.

  17. Carbon isotope effects associated with aceticlastic methanogenesis

    NASA Technical Reports Server (NTRS)

    Gelwicks, J. T.; Risatti, J. B.; Hayes, J. M.

    1994-01-01

    The carbon isotope effects associated with synthesis of methane from acetate have been determined for Methanosarcina barkeri 227 and for methanogenic archaea in sediments of Wintergreen Lake, Michigan. At 37 degrees C, the 13C isotope effect for the reaction acetate (methyl carbon) --> methane, as measured in replicate experiments with M. barkeri, was - 21.3% +/- 0.3%. The isotope effect at the carboxyl portion of acetate was essentially equal, indicating participation of both positions in the rate-determining step, as expected for reactions catalyzed by carbon monoxide dehydrogenase. A similar isotope effect, - 19.2% +/- 0.3% was found for this reaction in the natural community (temperature = 20 degrees C). Given these observations, it has been possible to model the flow of carbon to methane within lake sediment communities and to account for carbon isotope compositions of evolving methane. Extension of the model allows interpretation of seasonal fluctuations in 13C contents of methane in other systems.

  18. Carbon isotope effects associated with aceticlastic methanogenesis.

    PubMed

    Gelwicks, J T; Risatti, J B; Hayes, J M

    1994-02-01

    The carbon isotope effects associated with synthesis of methane from acetate have been determined for Methanosarcina barkeri 227 and for methanogenic archaea in sediments of Wintergreen Lake, Michigan. At 37 degrees C, the 13C isotope effect for the reaction acetate (methyl carbon) --> methane, as measured in replicate experiments with M. barkeri, was - 21.3% +/- 0.3%. The isotope effect at the carboxyl portion of acetate was essentially equal, indicating participation of both positions in the rate-determining step, as expected for reactions catalyzed by carbon monoxide dehydrogenase. A similar isotope effect, - 19.2% +/- 0.3% was found for this reaction in the natural community (temperature = 20 degrees C). Given these observations, it has been possible to model the flow of carbon to methane within lake sediment communities and to account for carbon isotope compositions of evolving methane. Extension of the model allows interpretation of seasonal fluctuations in 13C contents of methane in other systems. PMID:11536629

  19. Device and method for separating oxygen isotopes

    DOEpatents

    Rockwood, Stephen D.; Sander, Robert K.

    1984-01-01

    A device and method for separating oxygen isotopes with an ArF laser which produces coherent radiation at approximately 193 nm. The output of the ArF laser is filtered in natural air and applied to an irradiation cell where it preferentially photodissociates molecules of oxygen gas containing .sup.17 O or .sup.18 O oxygen nuclides. A scavenger such as O.sub.2, CO or ethylene is used to collect the preferentially dissociated oxygen atoms and recycled to produce isotopically enriched molecular oxygen gas. Other embodiments utilize an ArF laser which is narrowly tuned with a prism or diffraction grating to preferentially photodissociate desired isotopes. Similarly, desired mixtures of isotopic gas can be used as a filter to photodissociate enriched preselected isotopes of oxygen.

  20. Carbon isotope effects associated with aceticlastic methanogenesis.

    PubMed Central

    Gelwicks, J T; Risatti, J B; Hayes, J M

    1994-01-01

    The carbon isotope effects associated with synthesis of methane from acetate have been determined for Methanosarcina barkeri 227 and for methanogenic archaea in sediments of Wintergreen Lake, Michigan. At 37 degrees C, the 13C isotope effect for the reaction acetate (methyl carbon) --> methane, as measured in replicate experiments with M. barkeri, was - 21.3% +/- 0.3%. The isotope effect at the carboxyl portion of acetate was essentially equal, indicating participation of both positions in the rate-determining step, as expected for reactions catalyzed by carbon monoxide dehydrogenase. A similar isotope effect, - 19.2% +/- 0.3% was found for this reaction in the natural community (temperature = 20 degrees C). Given these observations, it has been possible to model the flow of carbon to methane within lake sediment communities and to account for carbon isotope compositions of evolving methane. Extension of the model allows interpretation of seasonal fluctuations in 13C contents of methane in other systems. PMID:11536629

  1. Boron-isotope geochemistry. Doctoral thesis

    SciTech Connect

    Spivack, A.J.

    1986-01-01

    An investigation of the major aspects of the boron-isotope geochemical cycle was carried out. Particular emphasis was directed at developing a reproducible, high-precision method for the determination of boron isotope ratios in geologic materials and determining the processes that influence the boron-isotope composition of seawater. A method for the determination of the isotopic composition of boron by thermal ionization mass spectrometry of Cs/sub 2/B/sub 4/O/sub 7/ is described. Samples analyzed for boron content and isotopic composition included: seawater, unaltered mid-ocean ridge basalts (MORB), altered MORB (dredge and core samples), serpentinized periodotites, marine sediments, marine sedimentary pore waters, hydrothermally altered sediments, oceanic hydrothermal solutions, rainwater, river water and suspended sediments, island arc volcanics and a soil profile.

  2. Isotopic composition of gases from mud volcanoes

    SciTech Connect

    Valysaev, B.M.; Erokhin, V.E.; Grinchenko, Y.I.; Prokhorov, V.S.; Titkov, G.A.

    1985-09-01

    A study has been made of the isotopic composition of the carbon in methane and carbon dioxide, as well as hydrogen in the methane, in the gases of mud volcanoes, for all main mud volcano areas in the USSR. The isotopic composition of carbon and hydrogen in methane shows that the gases resemble those of oil and gas deposits, while carbon dioxide of these volcanoes has a heavier isotopic composition with a greater presence of ''ultraheavy'' carbon dioxide. By the chemical and isotopic composition of gases, Azerbaidzhan and South Sakhalin types of mud volcano gases have been identified, as well as Bulganak subtypes and Akhtala and Kobystan varieties. Correlations are seen between the isotopic composition of gases and the geological build of mud volcano areas.

  3. Atomic vapor laser isotope separation of lead-210 isotope

    DOEpatents

    Scheibner, Karl F.; Haynam, Christopher A.; Johnson, Michael A.; Worden, Earl F.

    1999-01-01

    An isotopically selective laser process and apparatus for removal of Pb-210 from natural lead that involves a one-photon near-resonant, two-photon resonant excitation of one or more Rydberg levels, followed by field ionization and then electrostatic extraction. The wavelength to the near-resonant intermediate state is counter propagated with respect to the second wavelength required to populate the final Rydberg state. This scheme takes advantage of the large first excited state cross section, and only modest laser fluences are required. The non-resonant process helps to avoid two problems: first, stimulated Raman Gain due to the nearby F=3/2 hyperfine component of Pb-207 and, second, direct absorption of the first transition process light by Pb-207.

  4. Atomic vapor laser isotope separation of lead-210 isotope

    DOEpatents

    Scheibner, K.F.; Haynam, C.A.; Johnson, M.A.; Worden, E.F.

    1999-08-31

    An isotopically selective laser process and apparatus for removal of Pb-210 from natural lead that involves a one-photon near-resonant, two-photon resonant excitation of one or more Rydberg levels, followed by field ionization and then electrostatic extraction. The wavelength to the near-resonant intermediate state is counter propagated with respect to the second wavelength required to populate the final Rydberg state. This scheme takes advantage of the large first excited state cross section, and only modest laser fluences are required. The non-resonant process helps to avoid two problems: first, stimulated Raman Gain due to the nearby F=3/2 hyperfine component of Pb-207 and, second, direct absorption of the first transition process light by Pb-207. 5 figs.

  5. Measured solubilities and speciations from oversaturation experiments of neptunium, plutonium, and americium in UE-25p No. 1 well water from the Yucca Mountain region: Milestone report 3329-WBS1.2.3.4.1.3.1

    SciTech Connect

    Nitsche, H.; Roberts, K.; Prussin, T.; Mueller, A.; Becraft, K.; Keeney, D.; Carpenter, S.A.; Gatti, R.C.

    1994-04-01

    Solubility and speciation are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are a part of predictive transport models. Results are presented from solubility and speciation experiments of {sup 237}NpO{sub 2}{sup +}, {sup 239}Pu{sup 4+}, and {sup 241}Am{sup 3+}/Nd{sup 3+} in a modified UE-25p No. 1 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at two different temperatures (25{degree} and 60{degree}C) and three pH values (6.0, 7.0, 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations significantly decreased with increasing temperature at pH 6 and 7. The concentration at pH 8.5 hardly decreased at all with increasing temperature. At both temperatures the concentrations were highest at pH 8.5, lowest at pH 7, and in between at pH 6. For the americium/neodymium solutions, the solubility decreased significantly with increasing temperature and increased somewhat with increasing pH.

  6. Measured solubilities and speciations of neptunium, plutonium, and americium in a typical groundwater (J-13) from the Yucca Mountain region; Milestone report 3010-WBS 1.2.3.4.1.3.1

    SciTech Connect

    Nitsche, H.; Gatti, R.C.; Standifer, E.M.

    1993-07-01

    Solubility and speciation data are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are part of predictive transport models. Results are presented from solubility and speciation experiments of {sup 237}NpO{sub 2}{sup +}, {sup 239}Pu{sup 4+}, {sup 241}Am{sup 3+}/Nd{sup 3+}, and {sup 243}Am{sup 3+} in J-13 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at three different temperatures (25{degree}, 60{degree}, and 90{degree}C) and pH values (5.9, 7.0, and 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations decreased with increasing temperature and showed no trend with pH. The americium solutions showed no clear solubility trend with increasing temperature and increasing pH.

  7. Apparatus for storing hydrogen isotopes

    DOEpatents

    McMullen, John W.; Wheeler, Michael G.; Cullingford, Hatice S.; Sherman, Robert H.

    1985-01-01

    An improved method and apparatus for storing isotopes of hydrogen (especially tritium) are provided. The hydrogen gas(es) is (are) stored as hydrides of material (for example uranium) within boreholes in a block of copper. The mass of the block is critically important to the operation, as is the selection of copper, because no cooling pipes are used. Because no cooling pipes are used, there can be no failure due to cooling pipes. And because copper is used instead of stainless steel, a significantly higher temperature can be reached before the eutectic formation of uranium with copper occurs, (the eutectic of uranium with the iron in stainless steel forming at a significantly lower temperature).

  8. Laser system for isotope separation

    NASA Astrophysics Data System (ADS)

    Shirayama, Shimpey; Mikatsura, Takefumi; Ueda, Hiroaki; Konagai, Chikara

    1990-06-01

    Atomic vapor laser isotope separation (AVLIS) is regarded as the most promising method to obtain srightly enriched economical nuclear fuel for a nuclear power plant. However, achieving a high power laser seems to be the bottle neck in its industrialization. In 1985, after successful development of high power lasers, the U.S. announced that AVLIS would be used for future methods of uranium enrichment. In Japan , Laser Atomic Separation Enrichment Research Associates of Japan (LASER-J), a joint Japanese utility companies research organization, was founded in April, 1987, to push a development program for laser uranium enrichment. Based on research results obtained from Japanese National Labs, and Universities , Laser-J is now constructing an AVLIS experimental facility at Tokai-mura. It is planned to have a 1-ton swu capacity per year in 1991. Previous to the experimental facility construction , Toshiba proceeded with the preliminary testing of an isotope separation system, under contract with Laser-J. Since the copper vapor laser (CVL) and the dye laser (DL) form a good combination , which can obtain high power tunable visible lights ,it is suitable to resonate uranium atoms. The laser system was built and was successfully operated in Toshiba for two years. The system consist of three copper vapor lasers , three dye lasers and appropriate o Atomic vapor laser isotope separation (AVLIS) is regarded as the most promising method to obtain srightly enriched economical nuclear fuel for a nuclear power plant. However, achieving a high power laser seems to be the bottle neck in its industrialization. In 1985, after successful development of high power lasers, the U.S. announced that AVLIS would be used for future methods of uranium enrichment. In Japan , Laser Atomic Separation Enrichment Research Associates of Japan (LASER-J) , a joint Japanese utility companies research organization , was founded in April, 1987, to push a development program for laser uranium enrichment

  9. Isotopic signatures by bulk analyses

    SciTech Connect

    Efurd, D.W.; Rokop, D.J.

    1997-12-01

    Los Alamos National Laboratory has developed a series of measurement techniques for identification of nuclear signatures by analyzing bulk samples. Two specific applications for isotopic fingerprinting to identify the origin of anthropogenic radioactivity in bulk samples are presented. The first example is the analyses of environmental samples collected in the US Arctic to determine the impact of dumping of radionuclides in this polar region. Analyses of sediment and biota samples indicate that for the areas sampled the anthropogenic radionuclide content of sediments was predominantly the result of the deposition of global fallout. The anthropogenic radionuclide concentrations in fish, birds and mammals were very low. It can be surmised that marine food chains are presently not significantly affected. The second example is isotopic fingerprinting of water and sediment samples from the Rocky Flats Facility (RFP). The largest source of anthropogenic radioactivity presently affecting surface-waters at RFP is the sediments that are currently residing in the holding ponds. One gram of sediment from a holding pond contains approximately 50 times more plutonium than 1 liter of water from the pond. Essentially 100% of the uranium in Ponds A-1 and A-2 originated as depleted uranium. The largest source of radioactivity in the terminal Ponds A-4, B-5 and C-2 was naturally occurring uranium and its decay product radium. The uranium concentrations in the waters collected from the terminal ponds contained 0.05% or less of the interim standard calculated derived concentration guide for uranium in waters available to the public. All of the radioactivity observed in soil, sediment and water samples collected at RFP was naturally occurring, the result of processes at RFP or the result of global fallout. No extraneous anthropogenic alpha, beta or gamma activities were detected. The plutonium concentrations in Pond C-2 appear to vary seasonally.

  10. Isotopic composition of Silurian seawater

    SciTech Connect

    Knauth, L.P.; Kealy, S.; Larimer, S.

    1985-01-01

    Direct isotopic analyses of 21 samples of the Silurian hydrosphere preserved as fluid inclusions in Silurian halite deposits in the Michigan Basin Salina Group yield delta/sup 18/O, deltaD ranging from 0.2 to +5.9 and -26 to -73, respectively. delta/sup 18/O has the same range as observed for modern halite facies evaporite waters and is a few per thousand higher than 100 analyses of fluid inclusions in Permian halite. deltaD is about 20 to 30 per thousand lower than modern and Permian examples. The trajectory of evaporating seawater on a deltaD-delta/sup 18/O diagram initially has a positive slope of 3-6, but hooks strongly downward to negative values, the shape of the hook depending upon humidity. Halite begins to precipitate at delta values similar to those observed for the most /sup 18/O rich fluid inclusions. Subsequent evaporation yields progressively more negative delta values as observed for the fluid inclusions. The fluid inclusion data can be readily explained in terms of evaporating seawater and are consistent with the degree of evaporation deduced from measured bromide profiles. These data are strongly inconsistent with arguments that Silurian seawater was 5.5 per thousand depleted in /sup 18/O. delta/sup 18/O for evaporite waters is systematically related to that of seawater, and does not show a -5.5 per thousand shift in the Silurian, even allowing for variables which affect the isotope evaporation trajectory. The lower deltaD may indicate a component of gypsum dehydration waters or may suggest a D-depleted Silurian hydrosphere.

  11. Isotopic yield in cold binary fission of even-even 244-258Cf isotopes

    NASA Astrophysics Data System (ADS)

    Santhosh, K. P.; Cyriac, Annu; Krishnan, Sreejith

    2016-05-01

    The cold binary fission of even-even 244-258Cf isotopes has been studied by taking the interacting barrier as the sum of Coulomb and proximity potential. The favorable fragment combinations are obtained from the cold valley plot (plot of driving potential vs. mass number of fragments) and by calculating the yield for charge minimized fragments. It is found that for 244,246,248Cf isotopes highest yield is for the fragments with isotope of Pb (Z = 82) as one fragment, whereas for 250Cf and 252Cf isotopes the highest yield is for the fragments with isotope of Hg (Z = 80) as one fragment. In the case of 254,256,258Cf isotopes the highest yield is for the fragments with Sn (Z = 50) as one fragment. Thus, the fragment combinations with maximum yield reveal the role of doubly magic and near doubly magic nuclei in binary fission. It is found that asymmetric splitting is favored for Cf isotopes with mass number A ≤ 250 and symmetric splitting is favored for Cf isotopes with A > 252. In the case of Cf isotope with A = 252, there is an equal probability for asymmetric and symmetric splitting. The individual yields obtained for the cold fission of 252Cf isotope are compared with the experimental data taken from the γ- γ- γ coincidences technique using Gammasphere.

  12. A carbon isotope mass balance for an anoxic marine sediment: Isotopic signatures of diagenesis

    NASA Technical Reports Server (NTRS)

    Boehme, Susan E.

    1993-01-01

    A carbon isotope mass balance was determined for the sediments of Cape Lookout Bight, NC to constrain the carbon budgets published previously. The diffusive, ebullitive and burial fluxes of sigma CO2 and CH4, as well as the carbon isotope signatures of these fluxes, were measured. The flux-weighted isotopic signature of the remineralized carbon (-18.9 plus or minus 2.7 per mil) agreed with the isotopic composition of the remineralized organic carbon determined from the particulate organic carbon (POC) delta(C-13) profiles (-19.2 plus or minus 0.2), verifying the flux and isotopic signature estimates. The measured delta(C-13) values of the sigma CO2 and CH4 diffusive fluxes were significantly different from those calculated from porewater gradients. The differences appear to be influenced by methane oxidation at the sediment-water interface, although other potential processes cannot be excluded. The isotope mass balance provides important information concerning the locations of potential diagenetic isotope effects. Specifically, the absence of downcore change in the delta(C-13) value of the POC fraction and the identical isotopic composition of the POC and the products of remineralization indicate that no isotopic fractionation is expressed during the initial breakdown of the POC, despite its isotopically heterogeneous composition.

  13. Nitrogen isotope fractionation during archaeal ammonia oxidation: Coupled estimates from isotopic measurements of ammonium and nitrite

    NASA Astrophysics Data System (ADS)

    Mooshammer, Maria; Stieglmeier, Michaela; Bayer, Barbara; Jochum, Lara; Melcher, Michael; Wanek, Wolfgang

    2014-05-01

    Ammonia-oxidizing archaea (AOA) are ubiquitous in marine and terrestrial environments and knowledge about the nitrogen (N) isotope effect associated with their ammonia oxidation activity will allow a better understanding of natural abundance isotope ratios, and therefore N transformation processes, in the environment. Here we examine the kinetic isotope effect for ammonia oxidation in a pure soil AOA culture (Ca. Nitrososphaera viennensis) and a marine AOA enrichment culture. We estimated the isotope effect from both isotopic signatures of ammonium and nitrite over the course of ammonia oxidation. Estimates of the isotope effect based on the change in the isotopic signature of ammonium give valuable insight, because these estimates are not subject to the same concerns (e.g., accumulation of an intermediate) as estimates based on isotopic measurements of nitrite. Our results show that both the pure soil AOA culture and a marine AOA enrichment culture have similar but substantial isotope effect during ammonia consumption (31-34 per mill; based on ammonium) and nitrite production (43-45 per mill; based on nitrite). The 15N fractionation factors of both cultures tested fell in the upper range of the reported isotope effects for archaeal and bacterial ammonia oxidation (10-41 per mill) or were even higher than those. The isotope fractionation for nitrite production was significantly larger than for ammonium consumption, indicating that (1) some intermediate (e.g., hydroxylamine) of ammonia oxidation accumulates, allowing for a second 15N fractionation step to be expressed, (2) a fraction of ammonia oxidized is lost via gaseous N forms (e.g., NO or N2O), which is 15N-enriched or (3) a fraction of ammonium is assimilated into AOA biomass, biomass becoming 15N-enriched. The significance of these mechanisms will be explored in more detail for the soil AOA culture, based on isotope modeling and isotopic measurements of biomass and N2O.

  14. Canadian Network for Isotopes in Precipitation (CNIP)and Isotope Climatology and Hydroclimatology in Canada

    NASA Astrophysics Data System (ADS)

    Birks, S. J.; Edwards, T. W.; Gibson, J. J.

    2002-12-01

    The distribution of stable isotopes in precipitation provides fundamental information about the partitioning of the global atmospheric water budget, and hence about key aspects of Earth's climate, that cannot be discerned using other means. Although continuing demand exists for monitoring of isotopes in precipitation to define isotopic input functions for local hydrologic studies or for calibration of isotopic indicators of paleoclimate, based on longterm averages and climatological norms, awareness is also growing of the significant value of the monthly snapshots of the precipitation isotope field provided by the IAEA/WMO Global Network for Isotopes in Precipitation and its affiliated national networks as benchmark maps of the ongoing and dynamic evolution of the global water cycle. An initiative within the Canadian Network for Isotopes in Precipitation program includes development of a spatial and temporal database incorporating Canadian data to create a gridded isotope overlay compatible with gridded pressure and flux field data from the NCAR/CDAS Re-analysis Project. This database includes interpolated fields of our current best approximations of climatological isotopic means in addition to the original monthly data for the period 1997-2000. Studies are underway to test the sensitivity of the isotope-climate signal in precipitation to changes in these parameters utilizing perturbations in local climate arising from the El Nino/Southern Oscillation (ENSO). Intriguing results have been obtained from preliminary studies incorporating pressure and flux field data for the 1997-98 El Nino with CNIP isotope overlays. The strongest climate anomalies were found during the winter following the 1997 El Nino event, consistent with the expected strengthening of the Pacific North American pattern during this period. Comparisons of the isotopic fields with climate fields illustrate the complexity and dynamic nature of isotope climate not evident in time-series of data from

  15. Oxygen Isotopes in the Terrestrial Planets

    NASA Astrophysics Data System (ADS)

    Clayton, R. N.

    2004-12-01

    Mechanisms that may account for oxygen isotope heterogeneity in meteorites on the microscopic scale do not seem adequate for explaining the similarities and differences in isotopic composition on a planetary scale. In chondrites, most of the isotopic variability can be attributed to photochemical enrichment of the two rare heavy isotopes with respect to the 16O-rich solar composition In the CO, CM, CI, and CR chondrites, an additional low-temperature aqueous alteration leads to mass-dependent further enrichment of the heavy isotopes. If the photochemical origin of the isotopic variation in chondrites is correct, then only a small fraction, represented primarily in CAIs, has the solar oxygen isotopic composition, and all other meteoritic components must have undergone photochemical processing. In addition, since the bulk isotopic compositions of the terrestrial planets and of the achondrite parent bodies are similar to those of chondrites, they too must be made of photochemically enriched matter. The photochemical reactions produce a non-equilibrium assemblage of gases, probably leading to a non-equilibrium assemblage of solids, particularly with respect to their oxidation state. These issues emphasize the importance of the measurement of oxygen isotopes in the Genesis solar wind mission. Within the Earth, oxygen isotope variations are due almost entirely to mass-dependent fractionation effects, giving a line of slope 0.52 on the three-isotope plot. The average crustal composition is 3 to 4 permil higher in delta-18O than the upper mantle. This difference is too large to be due to igneous fractionation effects alone, and reflects the larger, low-temperature isotope fractionation associated with aqueous weathering reactions at the Earth's surface. Similar effects are not observed in the intraplanetary isotopic variations in the Moon or in the parent bodies of the HED and SNC meteorites. The bulk oxygen isotopic compositions of Earth and Mars (assumed to be the SNC

  16. Isotope separation by photoselective dissociative electron capture

    DOEpatents

    Stevens, Charles G. [Pleasanton, CA

    1978-08-29

    A method of separating isotopes based on photoselective electron capture dissociation of molecules having an electron capture cross section dependence on the vibrational state of the molecule. A molecular isotope source material is irradiated to selectively excite those molecules containing a desired isotope to a predetermined vibrational state having associated therewith an electron capture energy region substantially non-overlapping with the electron capture energy ranges associated with the lowest vibration states of the molecules. The isotope source is also subjected to electrons having an energy corresponding to the non-overlapping electron capture region whereby the selectively excited molecules preferentially capture electrons and dissociate into negative ions and neutrals. The desired isotope may be in the negative ion product or in the neutral product depending upon the mechanism of dissociation of the particular isotope source used. The dissociation product enriched in the desired isotope is then separated from the reaction system by conventional means. Specifically, .sup.235 UF.sub.6 is separated from a UF.sub.6 mixture by selective excitation followed by dissociative electron capture into .sup.235 UF.sub.5 - and F.

  17. Isotope separation by photoselective dissociative electron capture

    DOEpatents

    Stevens, C.G.

    1978-08-29

    Disclosed is a method of separating isotopes based on photoselective electron capture dissociation of molecules having an electron capture cross section dependence on the vibrational state of the molecule. A molecular isotope source material is irradiated to selectively excite those molecules containing a desired isotope to a predetermined vibrational state having associated therewith an electron capture energy region substantially non-overlapping with the electron capture energy ranges associated with the lowest vibration states of the molecules. The isotope source is also subjected to electrons having an energy corresponding to the non-overlapping electron capture region whereby the selectively excited molecules preferentially capture electrons and dissociate into negative ions and neutrals. The desired isotope may be in the negative ion product or in the neutral product depending upon the mechanism of dissociation of the particular isotope source used. The dissociation product enriched in the desired isotope is then separated from the reaction system by conventional means. Specifically, [sup 235]UF[sub 6] is separated from a UF[sub 6] mixture by selective excitation followed by dissociative electron capture into [sup 235]UF[sub 5]- and F. 2 figs.

  18. Deconstructing nitrate isotope dynamics in aquifers

    NASA Astrophysics Data System (ADS)

    Granger, J.

    2012-12-01

    The natural abundance N and O stable isotope ratios of nitrate provide an invaluable tool to differentiate N sources to the environment, track their dispersal, and monitor their attenuation by biological transformations. The interpretation of patterns in isotope abundances relies on knowledge of the isotope ratios of the source end-members, as well as on constraints on the isotope discrimination imposed on nitrate by respective biological processes. Emergent observations from mono-culture experiments of denitrifying bacteria reveal nitrate fractionation trends that appear at odds with trends ascribed to denitrification in soils and aquifers. This discrepancy raises the possibility that additional biological N transformations may be acting in tandem with denitrification. Here, the N and O isotope enrichments associated with nitrate removal by denitrification in aquifers are posited to bear evidence of coincident biological nitrate production - from nitrification and/or from anammox. Simulations are presented from a simple time-dependent one-box model of a groundwater mass ageing that is subject to net nitrate loss by denitrification with coincident nitrate production by nitrification or anammox. Within boundary conditions characteristic of freshwater aquifers, the apparent slope of the parallel enrichments in nitrate N and O isotopes associated with net N loss to denitrification can vary in proportion to the nitrate added simultaneous by oxidative processes. Pertinent observations from nitrate plumes in suboxic to anoxic aquifers are examined to validate this premise. In this perspective, nitrate isotope distributions suggest that we may be missing important N fluxes inherent to most aquifers.

  19. Si isotope homogeneity of the solar nebula

    SciTech Connect

    Pringle, Emily A.; Savage, Paul S.; Moynier, Frédéric; Jackson, Matthew G.; Barrat, Jean-Alix E-mail: savage@levee.wustl.edu E-mail: moynier@ipgp.fr E-mail: Jean-Alix.Barrat@univ-brest.fr

    2013-12-20

    The presence or absence of variations in the mass-independent abundances of Si isotopes in bulk meteorites provides important clues concerning the evolution of the early solar system. No Si isotopic anomalies have been found within the level of analytical precision of 15 ppm in {sup 29}Si/{sup 28}Si across a wide range of inner solar system materials, including terrestrial basalts, chondrites, and achondrites. A possible exception is the angrites, which may exhibit small excesses of {sup 29}Si. However, the general absence of anomalies suggests that primitive meteorites and differentiated planetesimals formed in a reservoir that was isotopically homogenous with respect to Si. Furthermore, the lack of resolvable anomalies in the calcium-aluminum-rich inclusion measured here suggests that any nucleosynthetic anomalies in Si isotopes were erased through mixing in the solar nebula prior to the formation of refractory solids. The homogeneity exhibited by Si isotopes may have implications for the distribution of Mg isotopes in the solar nebula. Based on supernova nucleosynthetic yield calculations, the expected magnitude of heavy-isotope overabundance is larger for Si than for Mg, suggesting that any potential Mg heterogeneity, if present, exists below the 15 ppm level.

  20. Stable Isotope Evidence for Planetary Differentiation

    NASA Astrophysics Data System (ADS)

    Shahar, A.; Mao, W. L.; Schauble, E. A.; Caracas, R.; Reagan, M. M.; Gleason, A. E.

    2015-12-01

    Planetary differentiation occurred at high temperature and varying oxygen fugacity, on bodies with varying compositions and internal pressures. The specific conditions at which bodies differentiated and the chemical fingerprints left by differentiation can be investigated by measuring stable isotope ratios in natural samples. Much can be learned by combining those data with experiments that systematically investigate the chemical and physical conditions within differentiating bodies. In this talk we focus on one variable in particular that has not been well defined with respect to stable isotope fractionation: pressure. We will present new iron isotope data on how pressure affects isotope fractionation factors for a number of iron compounds relative to silicate. The processes governing iron isotope fractionation in igneous rocks have been debated extensively over the past decade. Analyses of natural samples show that iron isotopes are fractionated at both the whole rock and mineral scales. This fractionation has been interpreted to be a result of several processes including a possible signature of high pressure core formation. We have collected new high pressure synchrotron nuclear resonant inelastic x-ray scattering data from Sector 16-ID-D at the Advanced Photon Source on 57Fe enriched Fe, FeO, FeHx and Fe3C. Our data show clear trends with pressure implying that not only does pressure have an effect on the iron isotope beta factors but also a fractionation amongst the alloys. This suggests that depending on the light element in the core, there will be a different resulting signature in the iron isotope record. We will discuss the likelihood of different light elements in the core based on these results, as well as the theoretical predictions for the same phases. Finally, we will present the fractionation expected between metal and silicate at high pressure and high temperature in order to determine if core formation would indeed leave an isotopic signature in

  1. Pb isotopic heterogeneity in basaltic phenocrysts

    SciTech Connect

    Bryce, Julia G.; DePaolo, Donald J.

    2002-06-01

    The Pb isotopic compositions of phenocrystic phases in young basaltic lavas have been investigated using the Getty-DePaolo method (Getty S. J. and DePaolo D. J. [1995] Quaternary geochronology by the U-Th-Pb method. Geochim. Cosmochim. Acta 59, 3267 3272), which allows for the resolution of small isotopic differences. Phenocryst, matrix, and whole rock analyses were made on samples from the 17 Myr-old Imnaha basalts of the Columbia River Group, a zero-age MORB from the Mid-Atlantic Ridge, and a ca. 260 kyr-old tholeiite from Mount Etna. Plagioclase feldspar phenocrysts have low-(U, Th)/Pb, and in each sample the plagioclase has significantly lower 206Pb/207Pb and 208Pb/207Pb values than whole rock, matrix, and magnetite-rich separates. The Pb isotopic contrast between plagioclase and matrix/whole rock is found in three samples with varying grain sizes (0.5 2 cm for the Imnaha basalt and MORB and <1 mm for the Etna sample) from different tectonic settings, suggesting that these results are not unique. The isotopic contrasts are only slightly smaller in magnitude than the variations exhibited by whole rock samples from the region. The Imnaha basalts also have Sr isotopic heterogeneity evident only in plagioclase phenocrysts, but the MORB and Etna lavas do not. The isotopic heterogeneities reflect magma mixing, and indicate that isotopically diverse magmas were mixed together just prior to eruption. The results reinforce indications from melt inclusion studies that magma source region isotopic heterogeneities have large amplitudes at short length scales, and that the isotopic variations imparted to the magmas are not entirely homogenized during segregation and transport processes.

  2. Stable isotope composition of Earth's large lakes

    NASA Astrophysics Data System (ADS)

    Jasechko, S.; Gibson, J. J.; YI, Y.; Birks, S. J.; Sharp, Z. D.

    2011-12-01

    Lakes cover about three percent of Earth's continental area. Large lakes can significantly influence lake shore and regional climates by increasing specific humidity during evaporation and by moderating air temperatures. Stable isotopes of oxygen and hydrogen can be used to quantify lake evaporation, providing a supplementary and often cost-advantageous alternative to conventional hydrologic approaches that require over lake monitoring. Further, stable isotopes in lake sediments are an established tool in paleolimnology; however, interpreting changes to a lake's past isotope composition requires a comprehensive understanding of contemporary controls. Here, δ18O and δ2H values of water in modern lakes exceeding roughly five hundred square kilometres are compiled (n > 35). Voluminous and seasonally mixed lakes - such as the North American Great Lakes - have the most homogenous stable isotope compositions, while perennially-stratified and shallow lakes show greater variability. A rudimentary stable isotope mass balance is used to assess evaporation fluxes from large lakes on Earth. The approach taken simultaneously constrains evaporation outputs for both oxygen and hydrogen stable isotopes by accounting for lake effects on the overlying atmosphere. Model development highlights important considerations such as isotopic stratification (Tanganyika), disequilibrium isotopic mass balances (Baikal), and non-steady hydrologic balances. Further, the isotope composition of Earth's continental surface water reservoir is calculated. This value - weighted to volume - is δ18O = -7.5±1.7 per mille relative to standard mean ocean water. The compiled data may be a useful tracer of continental evaporate in global atmospheric water cycle studies and could be coupled to climate models capable of incorporating oxygen-18 and deuterium tracers to improve or validate calculations of lake effects on regional water cycling.

  3. Isotopic CO2 Instrumentation for UAV Measurements

    NASA Astrophysics Data System (ADS)

    Gomez, A.; Silver, J.

    2013-12-01

    Carbon dioxide is the largest component of anthroprogenic green house gas emissions. Knowing atmospheric 13CO2/12CO2 ratios precisely is important for understanding biogenic and anthroprogenic sources and sinks for carbon. Instrumentation mounted on UAV aircraft would enable important spatial isotopic CO2 information. However, current isotopic CO2 instrumentation have unfavorable attributes for UAV use, such as high power requirements, high cost, high weight, and large size. Here we present the early development of a compact isotopic CO2 instrument that is designed to nullify effects of pressure, temperature and moisture, and will ultimately be suitable for UAV deployment.

  4. Isotopic Fractionation of Selenium Oxyanions in Wetlands

    NASA Astrophysics Data System (ADS)

    Clark, S. K.; Johnson, T. M.

    2004-05-01

    As oxic surface waters pass through aquatic macrophytes and over anoxic sediments in wetlands and lakes, the dissolved Se load often decreases; and, Se isotope ratio measurements can provide information about the mechanisms involved. Previous work on microbially induced isotopic fractionation of Se oxyanions under nearly natural conditions using wetland sediments shows consistent Se isotopic shifts during reduction of Se(VI) and Se(IV) to insoluble Se(0). However, previous isotopic studies of total dissolved selenium in wetlands found little to no isotopic shift as dissolved selenium concentrations decreased. This suggests that plant/algal uptake, followed by deposition and degradation, is the primary route of Se transfer into sediments. However, it is possible that the effective isotopic fractionation between Se in the surface water and Se deposited into sediments is somehow much less than the fractionation induced by the reduction reaction, or that cycling of organically bound Se is involved. In this study, we report Se isotope data for Se(VI), Se(IV) and total dissolved Se, Se(T), in surface waters from three wetland/lake sites: Sweitzer Lake, CO; 33-Mile Reservoir, WY; and, a small pond adjacent to Benton Lake, MT. We isolated Se(IV) via hydride generation, and Se(VI) via ion exchange. Se(T), including any organic components, was also analyzed. Isotope analysis was performed on an Isoprobe MC-ICPMS, using a method modified from that of Rouxel et al. (2002). We used the 82Se + 74Se double spike approach, and spiked samples before species separation. Our results for all three locations indicate similar trends in concentration changes and isotopic shifts between the inflow and outflow waters. Se(T) concentrations decrease by 45-70%, and Se(VI) concentrations decrease by 60-90%, whereas Se(IV) concentrations increase by 60-150%. Concomitant 80Se/76Se shifts are +0.5-0.8‰ for Se(T); -0.1-0.5‰ for Se(VI); and +0.4-6.5‰ for Se(IV). These data provide greater

  5. Theory of the Helium Isotope Shift

    SciTech Connect

    Pachucki, Krzysztof; Yerokhin, V. A.

    2015-09-15

    Theory of the isotope shift of the centroid energies of light few-electron atoms is reviewed. Numerical results are presented for the isotope shift of the 2{sup 3}P-2{sup 3}S and 2{sup 1}S-2{sup 3}S transition energies of {sup 3}He and {sup 4}He. By comparing theoretical predictions for the isotope shift with the experimental results, the difference of the squares of the nuclear charge radii of {sup 3}He and {sup 4}He, δR{sup 2}, is determined with high accuracy.

  6. Isotope effects on desorption kinetics of hydrogen isotopes implanted into stainless steel by glow discharge

    SciTech Connect

    Matsuyama, M.; Kondo, M.; Noda, N.; Tanaka, M.; Nishimura, K.

    2015-03-15

    In a fusion device the control of fuel particles implies to know the desorption rate of hydrogen isotopes by the plasma-facing materials. In this paper desorption kinetics of hydrogen isotopes implanted into type 316L stainless steel by glow discharge have been studied by experiment and numerical calculation. The temperature of a maximum desorption rate depends on glow discharge time and heating rate. Desorption spectra observed under various experimental conditions have been successfully reproduced by numerical simulations that are based on a diffusion-limited process. It is suggested, therefore, that desorption rate of a hydrogen isotope implanted into the stainless steel is limited by a diffusion process of hydrogen isotope atoms in bulk. Furthermore, small isotope effects were observed for the diffusion process of hydrogen isotope atoms. (authors)

  7. Short course on St-02 applications of isotope dilutions and isotopic measurements

    SciTech Connect

    Miller, P.

    1998-01-05

    This short course includes information on these topics and subtopics: (I) Nuclear Properties: (A) Historic roots; (B) Nomenclature; (C) Nuclear Stability and abundance; (D) Uses of isotopic techniques; (II) Instrumentation: (A) Sources; (B) Mass resolving elements; (C) Detectors; (III) Making Isotopic Measurements by ICP-MS: (A) Deadtime Correction; (B) Mass Discrimination; (C) Signal /Noise considerations; (IV) Applications and examples: (A) Isotope dilution; (B) Double Spike; (C) Biological Application; (D) Environmental Application; (E) Geological.

  8. Synthetic isotope mixtures for the calibration of isotope amount ratio measurements of carbon

    NASA Astrophysics Data System (ADS)

    Russe, K.; Valkiers, S.; Taylor, P. D. P.

    2004-07-01

    Synthetic isotope mixtures for the calibration of carbon isotope amount ratio measurements have been prepared by mixing carbon tetrafluoride highly enriched in 13C with carbon tetrafluoride depleted in 13C. Mixing procedures based on volumetry and gravimetry are described. The mixtures served as primary measurement standards for the calibration of isotope amount ratio measurements of the Isotopic Reference Materials PEF1, NBS22 and USGS24. Thus SI-traceable measurements of absolute carbon isotope amount ratios have been performed for the first time without any hypothesis needed for a correction of oxygen isotope abundances, such as is the case for measurements on carbon dioxide. As a result, "absolute" carbon isotope amount ratios determined via carbon tetrafluoride have smaller uncertainties than those published for carbon dioxide. From the measurements of the Reference Materials concerned, the absolute carbon isotope amount ratio of Vienna Pee Dee Belemnite (VPDB)--the hypothetical material upon which the scale for relative carbon isotope ratio measurements is based--was calculated to be R13(VPDB) = (11 101 +/- 16) × 10-6.

  9. Isotope pattern deconvolution as rising tool for isotope tracer studies in environmental research

    NASA Astrophysics Data System (ADS)

    Irrgeher, Johanna; Zitek, Andreas; Prohaska, Thomas

    2014-05-01

    During the last decade stable isotope tracers have emerged as versatile tool in ecological research. Besides 'intrinsic' isotope tracers caused by the natural variation of isotopes, the intentional introduction of 'extrinsic' enriched stable isotope tracers into biological systems has gained significant interest. Hereby the induced change in the natural isotopic composition of an element allows amongst others for studying the fate and fluxes of metals, trace elements and species in organisms or provides an intrinsic marker or tag of particular biological samples. Due to the shoreless potential of this methodology, the number of publications dealing with applications of isotope (double) spikes as tracers to address research questions in 'real world systems' is constantly increasing. However, some isotope systems like the natural Sr isotopic system, although potentially very powerful for this type of application, are still rarely used, mainly because their adequate measurement/determination poses major analytical challenges; as e.g. Sr is available in significant amounts in natural samples. In addition, biological systems underlie complex processes such as metabolism, adsorption/desorption or oxidation/reduction. As a consequence, classic evaluation approaches such as the isotope dilution mass spectrometry equation are often not applicable because of the unknown amount of tracer finally present in the sample. Isotope pattern deconvolution (IPD), based on multiple linear regression, serves as simplified alternative data processing strategy to double spike isotope dilution calculations. The outstanding advantage of this mathematical tool lies in the possibility of deconvolving the isotope pattern in a spiked sample without knowing the quantities of enriched isotope tracer being incorporated into the natural sample matrix as well as the degree of impurities and species-interconversion (e.g. from sample preparation). Here, the potential of IPD for environmental tracer

  10. Evaluating chlorine isotope effects from isotope ratios and mass spectra of polychlorinated molecules.

    PubMed

    Elsner, Martin; Hunkeler, Daniel

    2008-06-15

    Compound-specific chlorine isotope analysis receives much interest to assess the fate of chlorinated hydrocarbons in contaminated environments. This paper provides a theoretical basis to calculate isotope ratios and quantify isotope fractionation from ion-current ratios of molecular- and fragment-ion multiplets. Because both (35)Cl and (37)Cl are of high abundance, polychlorinated hydrocarbons consist of molecules containing different numbers of (37)Cl denoted as isotopologues. We show that, during reactions, the changes in isotopologue ratios are proportional to changes in the isotope ratio assuming a nonselective isotope distribution in the initial compound. This proportionality extents even to fragments formed in the ion source of a mass spectrometer such as C 2Cl 2 (double dechlorinated fragment of perchloroethylene, PCE). Fractionation factors and kinetic isotope effects (KIE) may, therefore, be evaluated from isotope, isotopologue or even fragment ratios according to conventional simple equations. The proportionality is exact with symmetric molecules such as dichloroethylene (DCE) and PCE, whereas it is approximately true with molecules containing nonreactive positions such as trichloroethylene (TCE). If in the latter case isotope ratios are derived from dechlorinated fragments, e.g., C 2HCl 2, it is important that fragmentation in the ion source affect all molecular positions alike, as otherwise isotopic changes in reactive positions may be underrepresented. PMID:18484745

  11. Variation in Atmospheric Helium Isotopes

    NASA Astrophysics Data System (ADS)

    Mabry, J. C.; Marty, B.; Burnard, P.; Blard, P.

    2010-12-01

    Anthropogenic activity such as oil and gas exploitation releases crustal helium, which has excess 4He compared to atmospheric helium. This may give rise to both spatial and temporal variations in the atmospheric 3He/4He. Helium is present in trace quantities in the air (5 ppm) and has a very low ratio (3He/4Heair = 1.38 x 10-6), consequently high precision measurements of atmospheric He presents a significant analytical challenge. Recent work by Sano et al. [1] has endeavored to experimentally quantify these potential variations in the atmospheric 3He/4He by measuring the helium isotopes from air samples collected around the globe and from samples of ancient trapped atmosphere. Their results indicate an increase in the atmospheric 3He/4He from northern to southern latitudes of the order 2 - 4 ‰, which they attribute to greater use of fossil fuels in the northern hemisphere. However, since most of their data points overlap at the 2-3 ‰ (2σ) level, additional measurements (with increased precision if possible) are needed. We have constructed an automated extraction line dedicated to measuring He in samples of air which can rapidly switch between measuring aliquots of sample with standards. It additionally features an adjustable bellows on the sample aliquot volume that enables us to adjust the size of a sample aliquot to precisely match the standard, eliminating biases arising from nonlinear pressure effects in the mass spectrometer. The measurements are made using a Helix SFT multi-collector mass spectrometer. At present, repeat measurements of 3He/4He from our standard (purified air) have a reproducibility of 2‰ (2σ), while measurements of local (Nancy, France) air samples have a reproducibility of 3He/4He of 3‰ (2σ), which are at a similar level to the uncertainties reported by Sano. Modifications are underway to improve 3He measurements which are the principal source of error. We have collected atmospheric samples from around the globe over a wide

  12. The seawater Sr isotopic evolution

    NASA Astrophysics Data System (ADS)

    Kuznetsov, A. B.; Gorokhov, I. M.; Semikhatov, M. A.; Maslov, A. V.; Krupenin, M. T.; Melnikov, N. N.

    2003-04-01

    Progress toward a reconstruction of the 87Sr/86Sr variations in Proterozoic seawater is still deficient compared to the Phanerozoic. There is no universally recognized curve, and some of its versions are in conflict. The construction of a reference curve should be based on: (1) the study of several thick carbonate-bearing successions within single paleobasin, (2) the reliable isotope dating of these successions, (3) the geochemical screening of least-altered carbonate samples, (4) a selective dissolution of samples to enrich them in primary carbonate generations. This approach was applied to study Late Proterozoic marine carbonate successions of the South Urals and East Siberia. Three comprehensive fragments of 87Sr/86Sr seawater curve were obtained: (1) the descending trend from 0.70562-0.70596 to 0.70519-0.70523 at 1050-1000 Ma, (2) the ascending trend from 0.70525-0.70535 to 0.70611-70625 at 850-750 Ma, and (3) the area of minor fluctuations from 0.70540 to 0.70610 at 680-660 Ma. The Sr- and C-isotope data for the South Urals allow us to revise the current stratigraphic correlations and impose some constraints on the age of the classic Upper Proterozoic successions of North Canada (Shaler Gr) and Svalbard (Akademikerbreen Gr): (1) the carbonate formations in middle part of the Shaler Gr appear to have been deposited after 800 Ma, (2) the rate of sedimentation of the Akademikerbreen succession was likely to be higher than it was proposed. The data from East Siberia postulate predominance of the low 87Sr/86Sr ratio during culmination stage of the Grenville orogenic cycle and decrease in this ratio in post-Grenvillian ocean. This fact markedly distinguishes the Grenville orogeny from the Pan-African orogeny which resulted in rise of seawater 87Sr/86Sr ratio up to 0.7085. The following factors were responsible for the low 87Sr/86Sr ratio in Grenvillian and post-Grenvillian oceans: a high role of mantle rocks in the exhumed orogens, a sea-level rise and partial

  13. Carbon isotope effects associated with autotrophic acetogenesis

    USGS Publications Warehouse

    Gelwicks, J.T.; Risatti, J.B.; Hayes, J.M.

    1989-01-01

    The carbon kinetic isotope effects associated with synthesis of acetate from CO2 and H2 during autotrophic growth of Acetobacterium woodii at 30??C have been measured by isotopic analyses of CO2, methyl-carbon, and total acetate. Closed systems allowing construction of complete mass balances at varying stages of growth were utilized, and the effects of the partitioning of carbon between CO2 and HCO3- were taken into account. For the overall reaction, total carbonate ??? total acetate, isotope effects measured in replicate experiments ranged from -59.0 ?? 0.9% to - 57.2 ?? 2.3z%. Taking into account all measurements, the weighted mean and standard deviation are -58.6 ?? 0.7%. There is no evidence for intramolecular ordering in the acetate. The carbon isotopic composition of sedimentary acetate, otherwise expected to be near that of sedimentary organic carbon, is likely to be depleted in environments in which autotrophic acetogenesis is occurring. ?? 1989.

  14. Applications of stable isotopes in clinical pharmacology

    PubMed Central

    Schellekens, Reinout C A; Stellaard, Frans; Woerdenbag, Herman J; Frijlink, Henderik W; Kosterink, Jos G W

    2011-01-01

    This review aims to present an overview of the application of stable isotope technology in clinical pharmacology. Three main categories of stable isotope technology can be distinguished in clinical pharmacology. Firstly, it is applied in the assessment of drug pharmacology to determine the pharmacokinetic profile or mode of action of a drug substance. Secondly, stable isotopes may be used for the assessment of drug products or drug delivery systems by determination of parameters such as the bioavailability or the release profile. Thirdly, patients may be assessed in relation to patient-specific drug treatment; this concept is often called personalized medicine. In this article, the application of stable isotope technology in the aforementioned three areas is reviewed, with emphasis on developments over the past 25 years. The applications are illustrated with examples from clinical studies in humans. PMID:21801197

  15. Water isotope systematics: Improving our palaeoclimate interpretations

    NASA Astrophysics Data System (ADS)

    Jones, M. D.; Dee, S.; Anderson, L.; Baker, A.; Bowen, G.; Noone, D. C.

    2016-01-01

    The stable isotopes of oxygen and hydrogen, measured in a variety of archives, are widely used proxies in Quaternary Science. Understanding the processes that control δ18O change have long been a focus of research (e.g. Shackleton and Opdyke, 1973; Talbot, 1990; Leng, 2006). Both the dynamics of water isotope cycling and the appropriate interpretation of geological water-isotope proxy time series remain subjects of active research and debate. It is clear that achieving a complete understanding of the isotope systematics for any given archive type, and ideally each individual archive, is vital if these palaeo-data are to be used to their full potential, including comparison with climate model experiments of the past. Combining information from modern monitoring and process studies, climate models, and proxy data is crucial for improving our statistical constraints on reconstructions of past climate variability.

  16. Isotope effects of hydrogen and atom tunnelling

    NASA Astrophysics Data System (ADS)

    Buchachenko, A. L.; Pliss, E. M.

    2016-06-01

    The abnormally high mass-dependent isotope effects in liquid-phase hydrogen (deuterium) atom transfer reactions, which are customarily regarded as quantum effects, are actually the products of two classical effects, namely, kinetic and thermodynamic ones. The former is determined by the rate constants for atom transfer and the latter is caused by nonbonded (or noncovalent) isotope effects in the solvation of protiated and deuterated reacting molecules. This product can mimic the large isotope effects that are usually attributed to tunnelling. In enzymatic reactions, tunnelling is of particular interest; its existence characterizes an enzyme as a rigid molecular machine in which the residence time of reactants on the reaction coordinate exceeds the waiting time for the tunnelling event. The magnitude of isotope effect becomes a characteristic parameter of the internal dynamics of the enzyme catalytic site. The bibliography includes 61 references.

  17. Atomic vapor laser isotope separation process

    DOEpatents

    Wyeth, R.W.; Paisner, J.A.; Story, T.

    1990-08-21

    A laser spectroscopy system is utilized in an atomic vapor laser isotope separation process. The system determines spectral components of an atomic vapor utilizing a laser heterodyne technique. 23 figs.

  18. Possible application of laser isotope separation

    NASA Technical Reports Server (NTRS)

    Delionback, L. M.

    1975-01-01

    The laser isotope separation process is described and its special economic features discussed. These features are its low cost electric power operation, capital investment costs, and the costs of process materials.

  19. The Palladium Isotopic Composition in Iron Meteorites

    NASA Technical Reports Server (NTRS)

    Chen, J. H.; Papanastassiou, D. A.

    2005-01-01

    Ru, Mo and Pd are very useful indicators for the identification of nucleosynthetic components. We have developed techniques for Pd isotopes, in an effort to check the extent of isotopic effects in this mass region and for a Pt-group element which is less refractory than Ru. Stable Pd isotopes are produced by the process only (102Pd), the s-process only (104Pd), the process only (Pd-110) and by both the r- and s-processes (Pd-105, Pd-106, Pd-108). Kelly and Wasserburg reported a hint of a shift in 102Pd (approx. 25(epsilon)u; 1(epsilon)u (triple bonds) 0.01%) in Santa Clara. Earlier searches for Mo and Ru isotopic anomalies were either positive or negative.

  20. Stable isotope investigations of chlorinated aliphatic hydrocarbons.

    SciTech Connect

    Abrajano, T.; Heraty, L. J.; Holt, B. D.; Huang, L.; Sturchio, N. C.

    1999-06-01

    Stable isotope ratio measurements for carbon (C) and chlorine (Cl) can be used to elucidate the processes affecting transformation and transportation of chlorinated aliphatic hydrocarbons (CAHs) in the environment. Methods recently developed in our laboratory for isotopic analysis of CAHs have been applied to laboratory measurements of the kinetic isotope effects associated with aerobic degradation of dichloromethane (DCM) and with both anaerobic and aerobic cometabolic degradation of trichlomethene (TCE) in batch and column microbial cultures. These experimental determinations of fractionation factors are crucial for understanding the behavior of CAHs in complex natural systems, where the extent of biotransformation can be masked by dispersion and volatilization. We have also performed laboratory investigations of kinetic isotope effects accompanying evaporation of CAHs, as well as field investigations of natural attenuation and in situ remediation of CAHs in a number of contaminated shallow aquifers at sites operated by the federal government and the private sector.

  1. Quantification of isotopic turnover in agricultural systems

    NASA Astrophysics Data System (ADS)

    Braun, A.; Auerswald, K.; Schnyder, H.

    2012-04-01

    The isotopic turnover, which is a proxy for the metabolic rate, is gaining scientific importance. It is quantified for an increasing range of organisms, from microorganisms over plants to animals including agricultural livestock. Additionally, the isotopic turnover is analyzed on different scales, from organs to organisms to ecosystems and even to the biosphere. In particular, the quantification of the isotopic turnover of specific tissues within the same organism, e.g. organs like liver and muscle and products like milk and faeces, has brought new insights to improve understanding of nutrient cycles and fluxes, respectively. Thus, the knowledge of isotopic turnover is important in many areas, including physiology, e.g. milk synthesis, ecology, e.g. soil retention time of water, and medical science, e.g. cancer diagnosis. So far, the isotopic turnover is quantified by applying time, cost and expertise intensive tracer experiments. Usually, this comprises two isotopic equilibration periods. A first equilibration period with a constant isotopic input signal is followed by a second equilibration period with a distinct constant isotopic input signal. This yields a smooth signal change from the first to the second signal in the object under consideration. This approach reveals at least three major problems. (i) The input signals must be controlled isotopically, which is almost impossible in many realistic cases like free ranging animals. (ii) Both equilibration periods may be very long, especially when the turnover rate of the object under consideration is very slow, which aggravates the first problem. (iii) The detection of small or slow pools is improved by large isotopic signal changes, but large isotopic changes also involve a considerable change in the input material; e.g. animal studies are usually carried out as diet-switch experiments, where the diet is switched between C3 and C4 plants, since C3 and C4 plants differ strongly in their isotopic signal. The

  2. Carbon isotopic fractionation in heterotrophic microbial metabolism

    NASA Technical Reports Server (NTRS)

    Blair, N.; Leu, A.; Munoz, E.; Olsen, J.; Kwong, E.; Des Marais, D.

    1985-01-01

    Differences in the natural-abundance carbon stable isotopic compositions between products from aerobic cultures of Escherichia coli K-12 were measured. Respired CO2 was 3.4 percent depleted in C-13 relative to the glucose used as the carbon source, whereas the acetate was 12.3 percent enriched in C-13. The acetate C-13 enrichment was solely in the carboxyl group. Even though the total cellular carbon was only 0.6 percent depleted in C-13, intracellular components exhibited a significant isotopic heterogeneity. The protein and lipid fractions were -1.1 and -2.7 percent, respectively. Aspartic and glutamic acids were -1.6 and +2.7 percent, respectively, yet citrate was isotopically identical to the glucose. Probable sites of carbon isotopic fractionation include the enzyme, phosphotransacetylase, and the Krebs cycle.

  3. Zinc Isotope Anomalies in bulk Chondrites

    NASA Astrophysics Data System (ADS)

    Savage, P. S.; Boyet, M.; Moynier, F.

    2014-09-01

    This study is the first to demonstrate that Zn isotope anomalies are present in bulk primitive meteorites, consistent with the injection of material derived from a neutron-rich supernova source into the solar nebula.

  4. Barium Isotopes in Single Presolar Grains

    NASA Technical Reports Server (NTRS)

    Pellin, M. J.; Davis, A. M.; Savina, M. R.; Kashiv, Y.; Clayton, R. N.; Lewis, R. S.; Amari, S.

    2001-01-01

    Barium isotopic compositions of single presolar grains were measured by laser ablation laser resonant ionization mass spectrometry and the implications of the data for stellar processes are discussed. Additional information is contained in the original extended abstract.

  5. Carbon isotopic fractionation in heterotrophic microbial metabolism.

    PubMed Central

    Blair, N; Leu, A; Muñoz, E; Olsen, J; Kwong, E; Des Marais, D

    1985-01-01

    Differences in the natural-abundance carbon stable isotopic compositions between products from aerobic cultures of Escherichia coli K-12 were measured. Respired CO2 was 3.4% depleted in 13C relative to the glucose used as the carbon source, whereas the acetate was 12.3% enriched in 13C. The acetate 13C enrichment was solely in the carboxyl group. Even though the total cellular carbon was only 0.6% depleted in 13C, intracellular components exhibited a significant isotopic heterogeneity. The protein and lipid fractions were -1.1 and -2.7%, respectively. Aspartic and glutamic acids were -1.6 and +2.7%, respectively, yet citrate was isotopically identical to the glucose. Probable sites of carbon isotopic fractionation include the enzyme, phosphotransacetylase, and the Krebs cycle. PMID:2867741

  6. Mercury Isotopes in Earth and Environmental Sciences

    NASA Astrophysics Data System (ADS)

    Blum, Joel D.; Sherman, Laura S.; Johnson, Marcus W.

    2014-05-01

    Virtually all biotic, dark abiotic, and photochemical transformations of mercury (Hg) produce Hg isotope fractionation, which can be either mass dependent (MDF) or mass independent (MIF). The largest range in MDF is observed among geological materials and rainfall impacted by anthropogenic sources. The largest positive MIF of Hg isotopes (odd-mass excess) is caused by photochemical degradation of methylmercury in water. This signature is retained through the food web and measured in all freshwater and marine fish. The largest negative MIF of Hg isotopes (odd-mass deficit) is caused by photochemical reduction of inorganic Hg and has been observed in Arctic snow and plant foliage. Ratios of MDF to MIF and ratios of 199Hg MIF to 201Hg MIF are often diagnostic of biogeochemical reaction pathways. More than a decade of research demonstrates that Hg isotopes can be used to trace sources, biogeochemical cycling, and reactions involving Hg in the environment.

  7. Nucleosynthesis and the Isotopic Composition of Stardust

    NASA Technical Reports Server (NTRS)

    Tielens, Alexander G. M.

    1997-01-01

    Various components have been isolated from carbonaceous meteorites with an isotopically anomalous elemental composition. Several of these are generally thought to represent stardust containing a nucleosynthetic record of their birthsites. This paper discusses the expected isotopic composition of stardust based upon astronomical observations and theoretical studies of their birthsites: red giants and supergiants, planetary nebulae, C-rich Wolf-Rayet stars, novae and supernovae. Analyzing the stardust budget, it is concluded that about 15% of the elements will be locked up in stardust components in the interstellar medium. This stardust will be isotopically heterogenous on an individual grain basis by factors ranging from 2 to several orders of magnitude. Since comets may have preserved a relatively unprocessed record of the stardust entering the solar nebula, isotopic studies of returned comet samples may provide valuable information on the nucleosynthetic processes taking place in the interiors of stars and the elemental evolution of the Milky Way.

  8. Carbon isotope effects associated with autotrophic acetogenesis.

    PubMed

    Gelwicks, J T; Risatti, J B; Hayes, J M

    1989-01-01

    The carbon kinetic isotope effects associated with synthesis of acetate from CO2 and H2 during autotrophic growth of Acetobacterium woodii at 30 degrees C have been measured by isotopic analyses of CO2, methyl-carbon, and total acetate. Closed systems allowing construction of complete mass balances at varying stages of growth were utilized, and the effects of the partitioning of carbon between CO2 and HCO3- were taken account. For the overall reaction, total carbonate --> total acetate, isotope effects measured in replicate experiments ranged from -59.0 +/- 0.9% to -57.2 +/- 2.3%. Taking into account all measurements, the weighted mean and standard deviation are -58.6 +/- 0.7%. There is no evidence for intramolecular ordering in the acetate. The carbon isotopic composition of sedimentary acetate, otherwise expected to be near that of sedimentary organic carbon, is likely to be depleted in environments in which autotrophic acetogenesis is occurring. PMID:11542159

  9. Carbon isotope effects associated with autotrophic acetogenesis

    NASA Technical Reports Server (NTRS)

    Gelwicks, J. T.; Risatti, J. B.; Hayes, J. M.

    1989-01-01

    The carbon kinetic isotope effects associated with synthesis of acetate from CO2 and H2 during autotrophic growth of Acetobacterium woodii at 30 degrees C have been measured by isotopic analyses of CO2, methyl-carbon, and total acetate. Closed systems allowing construction of complete mass balances at varying stages of growth were utilized, and the effects of the partitioning of carbon between CO2 and HCO3- were taken account. For the overall reaction, total carbonate --> total acetate, isotope effects measured in replicate experiments ranged from -59.0 +/- 0.9% to -57.2 +/- 2.3%. Taking into account all measurements, the weighted mean and standard deviation are -58.6 +/- 0.7%. There is no evidence for intramolecular ordering in the acetate. The carbon isotopic composition of sedimentary acetate, otherwise expected to be near that of sedimentary organic carbon, is likely to be depleted in environments in which autotrophic acetogenesis is occurring.

  10. Carbon isotopic fractionation in heterotrophic microbial metabolism

    SciTech Connect

    Blair, N.; Leu, A.; Munoz, E.; Olsen, J.; Kwong, E.; Des Marais, D.

    1985-10-01

    Differences in the natural-abundance carbon stable isotopic compositions between products from aerobic cultures of Escherichia coli K-12 were measured. Respired CO2 was 3.4 percent depleted in C-13 relative to the glucose used as the carbon source, whereas the acetate was 12.3 percent enriched in C-13. The acetate C-13 enrichment was solely in the carboxyl group. Even though the total cellular carbon was only 0.6 percent depleted in C-13, intracellular components exhibited a significant isotopic heterogeneity. The protein and lipid fractions were -1.1 and -2.7 percent, respectively. Aspartic and glutamic acids were -1.6 and +2.7 percent, respectively, yet citrate was isotopically identical to the glucose. Probable sites of carbon isotopic fractionation include the enzyme, phosphotransacetylase, and the Krebs cycle. 38 references.

  11. Photodisintegration of the isotope {sup 116}Cd

    SciTech Connect

    Belyshev, S. S.; Ishkhanov, B. S.; Orlin, V. N.; Stopani, K. A.; Khankin, V. V.; Shvedunov, N. V.

    2013-08-15

    The results obtained by measuring the yields of photodisintegration of the isotope {sup 116}Cd irradiated with bremsstrahlung photons whose spectrum had an endpoint energy of 55 MeV are presented and compared with the results of theoretical calculations.

  12. Magnesium isotopic composition of the mantle

    NASA Astrophysics Data System (ADS)

    Teng, F.; Li, W.; Ke, S.; Marty, B.; Huang, S.; Dauphas, N.; Wu, F.; Helz, R. L.

    2009-12-01

    Studies of Mg isotopic composition of the Earth not only are important for understanding its geochemistry but also can shed light on the accretion history of the Earth as well as the evolution of the Earth-Moon system. However, to date, the Mg isotopic composition of the Earth is still poorly constrained and highly debated. There is uncertainty in the magnitude of Mg isotope fractionation at mantle temperatures and whether the Earth has a chondritic Mg isotopic composition or not. To constrain further the Mg isotopic composition of the mantle and investigate the behavior of Mg isotopes during igneous differentiation, we report >200 high-precision (δ26Mg < 0.1‰, 2SD) analyses of Mg isotopes on 1) global mid-ocean ridge basalts covering major ridge segments of the world and spanning a broad range in latitudes, chemical and radiogenic isotopic compositions; 2) ocean island basalts from Hawaiian (Koolau, Kilauea and Loihi) and French Polynesian volcanoes (Society island and Cook Austral chain); 3) olivine grains from Hawaiian volcanoes (Kilauea, Koolau and Loihi) and 4) peridotite xenoliths from Australia, China, France, Tanzania and USA. Global oceanic basalts and peridotite xenoliths have a limited (<0.2 ‰) variation in Mg isotopic composition, with an average δ26Mg = -0.25 relative to DSM3. Olivines from Hawaiian lavas have δ26Mg ranging from -0.43 to +0.03, with most having compositions identical to basalts and peridotites. Therefore, the mantle’s δ26Mg value is estimated to be ~ -0.25 ± 0.1 (2SD), different from that reported by Wiechert and Halliday (2007; δ26Mg = ~ 0) but similar to more recent studies (δ26Mg = -0.27 to -0.33) (Teng et al. 2007; Handler et al. 2009; Yang et al., 2009). Moreover, we suggest the Earth, as represented by the mantle, has a Mg isotopic composition similar to chondrites (δ26Mg = ~-0.33). The need for a model such as that of Wiechert and Halliday (2007) that involves sorting of chondrules and calcium

  13. Isotopic fractionation of zinc in tektites

    NASA Astrophysics Data System (ADS)

    Moynier, Frederic; Beck, Pierre; Jourdan, Fred; Yin, Qing-Zhu; Reimold, Uwe; Koeberl, Christian

    2009-01-01

    Tektites are terrestrial natural glasses produced during a hypervelocity impact of an extraterrestrial projectile onto the Earth's surface. The similarity between the chemical and isotopic compositions of tektites and terrestrial upper continental crust implies that the tektites formed by fusion of such target rock. Tektites are among the driest rocks on Earth. Although volatilization at high temperature may have caused this extreme dryness, the exact mechanism of the water loss and the behavior of other volatile species during tektite formation are still debated. Volatilization can fractionate isotopes, therefore, comparing the isotope composition of volatile elements in tektites with that of their source rocks may help to understand the physical conditions during tektite formation. For this study, we have measured the Zn isotopic composition of 20 tektites from four different strewn fields. Almost all samples are enriched in heavy isotopes of Zn compared to the upper continental crust. On average, the different groups of tektites are isotopically distinct (listed from the isotopically lightest to the heaviest): Muong-Nong type indochinites ( δ66/64Zn = 0.61 ± 0.30‰); North American bediasites ( δ66/64Zn = 1.61 ± 0.49‰); Ivory Coast tektites ( δ66/64Zn = 1.66 ± 0.18‰); the Australasian tektites (others than the Muong Nong-type indochinites) ( δ66/64Zn = 1.84 ± 0.42‰); and Central European moldavites ( δ66/64Zn = 2.04 ± 0.19‰). These results are contrasted with a narrow range of δ66/64Zn = 0-0.7‰ for a diverse spectrum of upper continental crust materials. The elemental abundance of Zn is negatively correlated with δ66/64Zn, which may reflect that isotopic fractionation occurred by evaporation during the heating event upon tektite formation. Simple Rayleigh distillation predicts isotopic fractionations much larger than what is actually observed, therefore, such a model cannot account for the observed Zn isotope fractionation in tektites. We

  14. Sulfur Isotope Effects of Dissimilatory Sulfite Reductase

    PubMed Central

    Leavitt, William D.; Bradley, Alexander S.; Santos, André A.; Pereira, Inês A. C.; Johnston, David T.

    2015-01-01

    The precise interpretation of environmental sulfur isotope records requires a quantitative understanding of the biochemical controls on sulfur isotope fractionation by the principle isotope-fractionating process within the S cycle, microbial sulfate reduction (MSR). Here we provide the only direct observation of the major (34S/32S) and minor (33S/32S, 36S/32S) sulfur isotope fractionations imparted by a central enzyme in the energy metabolism of sulfate reducers, dissimilatory sulfite reductase (DsrAB). Results from in vitro sulfite reduction experiments allow us to calculate the in vitro DsrAB isotope effect in 34S/32S (hereafter, 34εDsrAB) to be 15.3 ± 2‰, 2σ. The accompanying minor isotope effect in 33S, described as 33λDsrAB, is calculated to be 0.5150 ± 0.0012, 2σ. These observations facilitate a rigorous evaluation of the isotopic fractionation associated with the dissimilatory MSR pathway, as well as of the environmental variables that govern the overall magnitude of fractionation by natural communities of sulfate reducers. The isotope effect induced by DsrAB upon sulfite reduction is a factor of 0.3–0.6 times prior indirect estimates, which have ranged from 25 to 53‰ in 34εDsrAB. The minor isotope fractionation observed from DsrAB is consistent with a kinetic or equilibrium effect. Our in vitro constraints on the magnitude of 34εDsrAB is similar to the median value of experimental observations compiled from all known published work, where 34εr−p = 16.1‰ (r–p indicates reactant vs. product, n = 648). This value closely matches those of MSR operating at high sulfate reduction rates in both laboratory chemostat experiments (34εSO4−H2S =  17.3 ± 1.5‰, 2σ) and in modern marine sediments (34εSO4−H2S =  17.3 ± 3.8‰). Targeting the direct isotopic consequences of a specific enzymatic processes is a fundamental step toward a biochemical foundation for reinterpreting the biogeochemical and geobiological sulfur isotope records in

  15. Diffusive Fractionation of Lithium Isotopes in Olivine

    NASA Astrophysics Data System (ADS)

    Homolova, V.; Richter, F. M.; Watson, E. B.; Chaussidon, M.

    2014-12-01

    Systematic lithium isotope variations along concentration gradients found in olivine and pyroxene grains from terrestrial, lunar and martian rocks have been attributed to diffusive isotopic fractionation [Beck et al., 2006; Tang et al., 2007]. In some cases, these isotopic excursions are so large that a single grain may display isotopic variability that spans almost the entire range of documented terrestrial values [Jeffcoate et al., 2007]. In this study, we present the results of experiments to examine diffusive isotopic fractionation of lithium in olivine. The experiments comprised crystallographically oriented slabs of San Carlos olivine juxtaposed with either spodumene powder or a lithium rich pyroxene crystal. Experiments were conducted at 1 GPa and 0.1MPa over a temperature range of 1000 to 1125⁰C. Oxygen fugacity in the 0.1MPa experiments was controlled using the wustite-magnetite and nickel-nickel oxide solid buffer assemblages. Lithium concentrations generally decrease smoothly away from the edges of the grains; however, experiments involving diffusion parallel to the a-axis consistently show peculiar wavy or segmented concentration profiles. Lithium diffusivity parallel to the c-axis is on the order of 1E-14m2/s at 1100⁰C. The diffusivity parallel to the c-axis is more than an order of magnitude faster than diffusion parallel to the b-axis and correlates positively with oxygen fugacity. The lithium isotopic composition, δ7Li = 1000‰ * ((δ7Lisample- δ7Ligrain center)/ δ7Ligrain center), shows a decrease away from the edge of the grain to a minimum value (up to 70‰ lighter) and then an abrupt increase back to the initial isotopic composition of the olivine grain. This isotopic profile is similar to those found in natural grains and an experimental study on diffusive fractionation of lithium isotopes in pyroxene [Richter et al., 2014]. Results from the present study are modeled using the approach of Dohmen et al. [2010], which assumes lithium

  16. Sulfur Isotope Effects of Dissimilatory Sulfite Reductase.

    PubMed

    Leavitt, William D; Bradley, Alexander S; Santos, André A; Pereira, Inês A C; Johnston, David T

    2015-01-01

    The precise interpretation of environmental sulfur isotope records requires a quantitative understanding of the biochemical controls on sulfur isotope fractionation by the principle isotope-fractionating process within the S cycle, microbial sulfate reduction (MSR). Here we provide the only direct observation of the major ((34)S/(32)S) and minor ((33)S/(32)S, (36)S/(32)S) sulfur isotope fractionations imparted by a central enzyme in the energy metabolism of sulfate reducers, dissimilatory sulfite reductase (DsrAB). Results from in vitro sulfite reduction experiments allow us to calculate the in vitro DsrAB isotope effect in (34)S/(32)S (hereafter, [Formula: see text]) to be 15.3 ± 2‰, 2σ. The accompanying minor isotope effect in (33)S, described as [Formula: see text], is calculated to be 0.5150 ± 0.0012, 2σ. These observations facilitate a rigorous evaluation of the isotopic fractionation associated with the dissimilatory MSR pathway, as well as of the environmental variables that govern the overall magnitude of fractionation by natural communities of sulfate reducers. The isotope effect induced by DsrAB upon sulfite reduction is a factor of 0.3-0.6 times prior indirect estimates, which have ranged from 25 to 53‰ in (34)εDsrAB. The minor isotope fractionation observed from DsrAB is consistent with a kinetic or equilibrium effect. Our in vitro constraints on the magnitude of [Formula: see text] is similar to the median value of experimental observations compiled from all known published work, where (34)ε r-p = 16.1‰ (r-p indicates reactant vs. product, n = 648). This value closely matches those of MSR operating at high sulfate reduction rates in both laboratory chemostat experiments ([Formula: see text] 17.3 ± 1.5‰, 2σ) and in modern marine sediments ([Formula: see text] 17.3 ± 3.8‰). Targeting the direct isotopic consequences of a specific enzymatic processes is a fundamental step toward a biochemical foundation for reinterpreting the

  17. Chromium stable isotope fractionation during adsorption

    NASA Astrophysics Data System (ADS)

    Ellis, A.; Johnson, T.; Bullen, T.

    2003-04-01

    Chromium is a common anthropogenic contaminant in ground water. It is redox-active; the two common valences in natural waters are Cr(VI), which is highly soluble and toxic, and Cr(III), which is relatively insoluble. Redox reactions control Cr mobility in aqueous solutions with Cr(VI) reduction to Cr(III) controlling the attenuation of Cr in groundwater. Our previous study demonstrated that abiotic Cr(VI) reduction causes an isotope fractionation of -3.5 permil (53Cr/52Cr) and isotopes can therefore be used to calculate the extent of reduction. In the present study, experiments were conducted to measure Cr isotope fractionation during Cr(VI) sorption on Al203. Sorption of Cr(VI) could be important as a small isotope fractionation may get amplified along the edges of a Cr(VI) contaminated plume. A previous study demonstrated a similar process with Fe isotopes on anion exchange resin. Initial solutions of 200 mg/l Cr(VI) (as K2Cr2O7) and 0.1 mM KCl were made up. Sufficient solid Al203 was added to achieve 50% sorption. After equilibration, the solution was extracted by centrifuging and filtering with a 0.2 micron filter. Al203 was then added again to result in a further 50% sorption of the remaining Cr(VI). This process was repeated 10 times to amplify any isotopic fractionation between dissolved and adsorbed Cr(VI). The instantaneous stable isotope fractionation was calculated based on the δ 53Cr values of the initial and final Cr(VI) solutions. The results show that the stable isotope values measured in the solutions after the ten steps were within the uncertainty of the isotope value of the initial solution. Therefore, no significant stable isotope fractionation occurred. We are presently conducting experiments with goethite and expect similar results. Therefore, any fractionation of chromium stable isotopes observed in contaminant plumes are a result of processes other than adsorption (i.e., reduction).

  18. Reactive transport modeling of Li isotope fractionation

    NASA Astrophysics Data System (ADS)

    Wanner, C.; Sonnenthal, E. L.

    2013-12-01

    The fractionation of Li isotopes has been used as a proxy for interaction processes between silicate rocks and any kind of fluids. In particular, Li isotope measurements are powerful because Li is almost exclusively found in silicate minerals. Moreover, the two stable Li isotopes, 6Li and 7Li, differ by 17% in mass introducing a large mass dependent isotope fractionation even at high temperature. Typical applications include Li isotope measurements along soil profiles and of river waters to track silicate weathering patterns and Li isotope measurements of geothermal wells and springs to assess water-rock interaction processes in geothermal systems. For this contribution we present a novel reactive transport modeling approach for the simulation of Li isotope fractionation using the code TOUGHREACT [1]. It is based on a 6Li-7Li solid solution approach similar to the one recently described for simulating Cr isotope fractionation [2]. Model applications include the simulation of granite weathering along a 1D flow path as well as the simulation of a column experiment related to an enhanced geothermal system. Results show that measured δ7Li values are mainly controlled by (i) the degree of interaction between Li bearing primary silicate mineral phases (e.g., micas, feldspars) and the corresponding fluid, (ii) the Li isotope fractionation factor during precipitation of secondary mineral phases (e.g., clays), (iii) the Li concentration in primary and secondary Li bearing mineral phases and (iv) the proportion of dissolved Li that adsorbs to negatively charged surfaces (e.g., clays, Fe/Al-hydroxides). To date, most of these parameters are not very well constrained. Reactive transport modeling thus currently has to rely on many assumptions. Nevertheless, such models are powerful because they are the only viable option if individual contributions of all potential processes on the resulting (i.e., measured) Li isotopic ratio have to be quantitatively assessed. Accordingly, we

  19. Isotopic quantum effects in liquid methanol.

    PubMed

    Ludwig, Ralf

    2005-07-11

    Density functional calculations (B3 LYP/6-31+G*) on molecular clusters and a quantum cluster equilibrium (QCE) model were used to calculate thermodynamic and structural properties of four isotopically labeled methanol species. The method allowed the reproduction of the characteristic differences in boiling points and heats of vaporization. Structural changes were also detected and related to recent experimental findings. It was shown that isotopic effects clearly have a quantum-mechanical origin. PMID:15991271

  20. Magnesium isotope geochemistry in arc volcanism

    PubMed Central

    Teng, Fang-Zhen; Hu, Yan

    2016-01-01

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ26Mg of the Martinique Island lavas varies from −0.25 to −0.10, in contrast to the narrow range that characterizes the mantle (−0.25 ± 0.04, 2 SD). These high δ26Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid−mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration. PMID:27303032

  1. Oxygen isotope relationships in iron meteorites

    NASA Technical Reports Server (NTRS)

    Clayton, R. N.; Mayeda, T. K.; Olsen, E. J.; Prinz, M.

    1983-01-01

    Iron meteorites with oxygen-bearing phases can be classified in terms of their oxygen isotopic abundances. These iron meteorite classes are isotopically similar to various stony meteorite classes, which may indicate a common origin. The group IAB and IIICD irons may be related to the winonaites; group IIE irons may be related to H chondrites; group IVA irons may be related to L or LL chondrites.

  2. Isotopic studies in returned lunar samples

    NASA Technical Reports Server (NTRS)

    Alexander, E. C., Jr.

    1971-01-01

    Analysis of lunar soil samples returned by Apollo 11 and 12 flights are discussed. Isotopic studies of the rare gases from Apollo 11 flight lunar samples are presented. The lunar soil analyses indicated the following: (1) high concentrations of solar wind rare gases, (2) isotopic match between solar wind gases and gas components in gas-rich meteorites, and (3) rare gases attributable to spallation reactions induced in heavier nuclides by cosmic ray particles.

  3. Isotope shortage triggers delays for patients

    NASA Astrophysics Data System (ADS)

    Gould, Paula

    2009-07-01

    An unplanned shutdown of a nuclear reactor in Canada is disrupting the supply of medical isotopes across North America and forcing some hospitals to cancel or postpone patients' tests. The closure of the National Research Universal (NRU) reactor in Chalk River, Ontario, has also embarrassed Canadian officials, including a senior government minister who was forced to apologize after calling the isotope shortage a "sexy" career challenge.

  4. IUPAC Periodic Table of the Isotopes

    USGS Publications Warehouse

    Holden, N.E.; Coplen, T.B.; Böhlke, J.K.; Wieser, M.E.; Singleton, G.; Walczyk, T.; Yoneda, S.; Mahaffy, P.G.; Tarbox, L.V.

    2011-01-01

    For almost 150 years, the Periodic Table of the Elements has served as a guide to the world of elements by highlighting similarities and differences in atomic structure and chemical properties. To introduce students, teachers, and society to the existence and importance of isotopes of the chemical elements, an IUPAC Periodic Table of the Isotopes (IPTI) has been prepared and can be found as a supplement to this issue.

  5. Magnesium isotope geochemistry in arc volcanism.

    PubMed

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine

    2016-06-28

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ(26)Mg of the Martinique Island lavas varies from -0.25 to -0.10, in contrast to the narrow range that characterizes the mantle (-0.25 ± 0.04, 2 SD). These high δ(26)Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid-mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration. PMID:27303032

  6. Magnesium isotope geochemistry in arc volcanism

    NASA Astrophysics Data System (ADS)

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine

    2016-06-01

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ26Mg of the Martinique Island lavas varies from ‑0.25 to ‑0.10, in contrast to the narrow range that characterizes the mantle (‑0.25 ± 0.04, 2 SD). These high δ26Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid‑mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration.

  7. Modeling Nitrogen Isotopes in the Global Ocean

    NASA Astrophysics Data System (ADS)

    Somes, C.; Schmittner, A.

    2008-12-01

    The nitrogen isotopic signal measured in marine sediments has the potential to be a valuable paleoceanographic proxy. It captures the response of different biological processes in the marine ecosystem including photosynthesis, nitrogen fixation, denitrification as well as processes within the food chain. A simple marine ecosystem model that includes the interactive cycling of nitrogen, phosphorus, and oxygen is augmented to record nitrogen isotopes in the University of Victoria Earth System Climate Model. New nitrogen isotopic tracers are employed at all trophic levels of the ecosystem. This includes the δ15N of nitrate, both classes of phytoplankton (nitrogen fixers and all other phytoplankton), zooplankton, and detritus. Despite a few shortcomings, it is shown that the nitrogen isotope model can capture the major trends observed in the modern climate. The ability to model nitrogen isotopes in a global coupled ocean- atmosphere-sea ice-ecosystem model gives us a unique opportunity to directly infer what physical and biological changes in the climate system are driving the δ15N signal on spatial and temporal scales. This is a valuable tool giving us tremendous insight on how to interpret the nitrogen isotopic signal.

  8. Iron isotopic systematics of oceanic basalts

    NASA Astrophysics Data System (ADS)

    Teng, Fang-Zhen; Dauphas, Nicolas; Huang, Shichun; Marty, Bernard

    2013-04-01

    The iron isotopic compositions of 93 well-characterized basalts from geochemically and geologically diverse mid-ocean ridge segments, oceanic islands and back arc basins were measured. Forty-three MORBs have homogeneous Fe isotopic composition, with δ56Fe ranging from +0.07‰ to +0.14‰ and an average of +0.105 ± 0.006‰ (2SD/√n, n = 43, MSWD = 1.9). Three back arc basin basalts have similar δ56Fe to MORBs. By contrast, OIBs are slightly heterogeneous with δ56Fe ranging from +0.05‰ to +0.14‰ in samples from Koolau and Loihi, Hawaii, and from +0.09‰ to +0.18‰ in samples from the Society Islands and Cook-Austral chain, French Polynesia. Overall, oceanic basalts are isotopically heavier than mantle peridotite and pyroxenite xenoliths, reflecting Fe isotope fractionation during partial melting of the mantle. Iron isotopic variations in OIBs mainly reflect Fe isotope fractionation during fractional crystallization of olivine and pyroxene, enhanced by source heterogeneity in Koolau samples.

  9. Gluconeogenesis from labeled carbon: estimating isotope dilution

    SciTech Connect

    Kelleher, J.K.

    1986-03-01

    To estimate the rate of gluconeogenesis from steady-state incorporation of labeled 3-carbon precursors into glucose, isotope dilution must be considered so that the rate of labeling of glucose can be quantitatively converted to the rate of gluconeogenesis. An expression for the value of this isotope dilution can be derived using mathematical techniques and a model of the tricarboxylic acid (TCA) cycle. The present investigation employs a more complex model than that used in previous studies. This model includes the following pathways that may affect the correction for isotope dilution: 1) flux of 3-carbon precursor to the oxaloacetate pool via acetyl-CoA and the TCA cycle; 2) flux of 4- or 5-carbon compounds into the TCA cycle; 3) reversible flux between oxaloacetate (OAA) and pyruvate and between OAA and fumarate; 4) incomplete equilibrium between OAA pools; and 5) isotope dilution of 3-carbon tracers between the experimentally measured pool and the precursor for the TCA-cycle OAA pool. Experimental tests are outlined which investigators can use to determine whether these pathways are significant in a specific steady-state system. The study indicated that flux through these five pathways can significantly affect the correction for isotope dilution. To correct for the effects of these pathways an alternative method for calculating isotope dilution is proposed using citrate to relate the specific activities of acetyl-CoA and OAA.

  10. Iron isotopic fractionation during continental weathering

    SciTech Connect

    Fantle, Matthew S.; DePaolo, Donald J.

    2003-10-01

    The biological activity on continents and the oxygen content of the atmosphere determine the chemical pathways through which Fe is processed at the Earth's surface. Experiments have shown that the relevant chemical pathways fractionate Fe isotopes. Measurements of soils, streams, and deep-sea clay indicate that the {sup 56}Fe/{sup 54}Fe ratio ({delta}{sup 56}Fe relative to igneous rocks) varies from +1{per_thousand} for weathering residues like soils and clays, to -3{per_thousand} for dissolved Fe in streams. These measurements confirm that weathering processes produce substantial fractionation of Fe isotopes in the modern oxidizing Earth surface environment. The results imply that biologically-mediated processes, which preferentially mobilize light Fe isotopes, are critical to Fe chemistry in weathering environments, and that the {delta}{sup 56}Fe of marine dissolved Fe should be variable and negative. Diagenetic reduction of Fe in marine sediments may also be a significant component of the global Fe isotope cycle. Iron isotopes provide a tracer for the influence of biological activity and oxygen in weathering processes through Earth history. Iron isotopic fractionation during weathering may have been smaller or absent in an oxygen-poor environment such as that of the early Precambrian Earth.

  11. Oxygen isotope studies of ordinary chondrites

    NASA Technical Reports Server (NTRS)

    Clayton, Robert N.; Mayeda, Toshiko K.; Olsen, Edward J.; Goswami, J. N.

    1991-01-01

    Several stages in the evolution of ordinary chondritic meteorites are recorded in the oxygen isotopic composition of the meteorites and their separable components (chondrules, fragments, clasts, and matrix). The whole-rock isotopic compositions reflect the iron-group of the meteorite (H, L, or LL). Isotopic uniformity of H3 to H6 and L3 to L6 are consistent with closed-system metamorphism within each parent body. LL3 chondrites differ slightly from LL4 to LL6, implying a small degree of open-system aqueous alteration and carbon reduction. On the scale of individual chondrules, the meteorites are isotopically heterogeneous, allowing recognition of the solar-nebular processes of chondrule formation. Chondrules for all classes of ordinary chondrites are derived from a common population, which was separate from the population of chondrules in carbonaceous or enstatite chondrites. Chondrules define an isotopic mixing line dominated by exchange between (O - 16)-rich and (O - 16)-poor reservoirs. The oxygen isotopic compositions of chondrites serve as 'fingerprints' for identification of genetic association with other meteorite types (achondrites and iron) and for recognition of source materials in meteoritic breccias.

  12. Isotopic tracing of perchlorate in the environment

    SciTech Connect

    Sturchio, N. C.; Bohlke, J. K.; Gu, Baohua; Hatzinger, Paul B.; Jackson, Andrew

    2011-01-01

    Isotopic data can be used for tracing the origin and behavior of ClO4- in the environment. Four independently varying parameters have been measured on individual ClO4- samples for this purpose: delta 37Cl, 18O, 17O, and 36Cl/Cl. At least three distinct types of ClO4- have been identified isotopically, and these distinctions have proven to be useful in forensic applications. Additional data for natural ClO4- are urgently needed, however, to obtain a global picture of its isotopic variations. Improved methods for sample preparation and isotopic analysis with much better sensitivity would be helpful for measuring ClO4- isotopic variations in some sample types such as aerosols and precipitation as well as foodstuffs and bodily fluids, which have been precluded by the impracticality of obtaining the currently-required milligram amounts of ClO4-.. Further experimental and theoretical investigations of atmospheric ClO4- production mechanisms may lead to improved explanations of observed isotopic variations in natural samples.

  13. Isotopic Dependence of GCR Fluence behind Shielding

    NASA Technical Reports Server (NTRS)

    Cucinotta, Francis A.; Wilson, John W.; Saganti, Premkumar; Kim, Myung-Hee Y.; Cleghorn, Timothy; Zeitlin, Cary; Tripathi, Ram K.

    2006-01-01

    In this paper we consider the effects of the isotopic composition of the primary galactic cosmic rays (GCR), nuclear fragmentation cross-sections, and isotopic-grid on the solution to transport models used for shielding studies. Satellite measurements are used to describe the isotopic composition of the GCR. For the nuclear interaction data-base and transport solution, we use the quantum multiple-scattering theory of nuclear fragmentation (QMSFRG) and high-charge and energy (HZETRN) transport code, respectively. The QMSFRG model is shown to accurately describe existing fragmentation data including proper description of the odd-even effects as function of the iso-spin dependence on the projectile nucleus. The principle finding of this study is that large errors (+/-100%) will occur in the mass-fluence spectra when comparing transport models that use a complete isotopic-grid (approx.170 ions) to ones that use a reduced isotopic-grid, for example the 59 ion-grid used in the HZETRN code in the past, however less significant errors (<+/-20%) occur in the elemental-fluence spectra. Because a complete isotopic-grid is readily handled on small computer workstations and is needed for several applications studying GCR propagation and scattering, it is recommended that they be used for future GCR studies.

  14. Isotopic composition of precipitation in Greece

    NASA Astrophysics Data System (ADS)

    Argiriou, Athanassios A.; Lykoudis, Spyros

    2006-08-01

    SummaryThe contribution of stable isotopes in meteorological, climatological and hydrological research is well known. Until this date and despite the fact that several hydrological studies of water sources in Greece have been published, no systematic isotopic study of precipitation has been performed in the country. This paper presents all the available isotopic data collected since 1960 in several Hellenic measurement stations. This data is divided in two periods: the first covers data that was collected in the past, in the frame of a preliminary survey of the isotope composition of precipitation in the Eastern Mediterranean Sea and specific hydrological studies; the second is the result of a three-year coordinated research project of the International Atomic Energy Agency, in which the authors participated, aiming at the systematic study of stable isotopes ( 2H and 18O) and 3H in precipitation around the Mediterranean basin. No statistically significant behavior between the two periods of data was found. The isotopic content of precipitation presents characteristics intermediate of those of the Eastern and Western Mediterranean. The tritium concentration in precipitation declines as expected towards the pre-bomb levels, however there is an indication that tritium concentrations are higher in Northern Greece.

  15. Grosnaja ABCs: Magnesium isotope compositions

    NASA Technical Reports Server (NTRS)

    Goswami, J. N.; Srinivasan, G.; Ulyanov, A. A.

    1993-01-01

    Three CAI's from the Grosnaja CV3 chondrite were analyzed for their magnesium isotopic compositions by the ion microprobe. The selected CAI's represent three distinct types: GR4(compact Type A), GR7(Type B) and GR2(Type C). Petrographic studies indicate that all three Grosnaja inclusions were subjected to secondary alterations. The Type A CAI GR4 is primarily composed of melilite with spinel and pyroxene occurring as minor phases. The rim of the inclusion does not exhibit distinct layered structure and secondary alteration products (garnet, Fe-rich olivine and Na-rich plagioclase) are present in some localized areas near the rim region. The average major element compositions of different mineral phases in GR4 are given. Preliminary REE data suggest a depletion of HREE relative to LREE by about a factor of 3 without any clear indication of interelement fractionation. The CAI GR7 has textural and minerological characteristics similar to Type B inclusions. The REE data show a pattern that is similar to Group 6 with enrichment in Eu and Yb. In addition, a depletion of HREE compared to LREE is also evident in this object. Melilite composition shows a broad range of akermanite content (Ak(sub 15-55)). Detailed petrographic study is in progress. GR2 is a anorthite-rich Type C inclusion with large plagioclase laths intergrown with Ti-rich pyroxene. The average plagioclase composition is close to pure anorthite (An99).

  16. Purdue Rare Isotope Measurement Laboratory

    NASA Astrophysics Data System (ADS)

    Caffee, M.; Elmore, D.; Granger, D.; Muzikar, P.

    2002-12-01

    The Purdue Rare Isotope Measurement Laboratory (PRIME Lab) is a dedicated research and service facility for accelerator mass spectrometry. AMS is an ultra-sensitive analytical technique used to measure low levels of long-lived cosmic-ray-produced and anthropogenic radionuclides, and rare trace elements. We measure 10Be (T1/2 = 1.5 My), 26Al (.702 My), 36Cl (.301 My), and 129I (16 My), in geologic samples. Applications include dating the cosmic-ray-exposure time of rocks on Earth's surface, determining rock and sediment burial ages, measuring the erosion rates of rocks and soils, and tracing and dating ground water. We perform sample preparation and separation chemistries for these radio-nuclides for our internal research activities and for those external researchers not possessing this capability. Our chemical preparation laboratories also serve as training sites for members of the geoscience community developing these techniques at their institutions. Research at Purdue involves collaborators among members of the Purdue Departments of Physics, Earth and Atmospheric Sciences, Chemistry, Agronomy, and Anthropology. We also collaborate and serve numerous scientists from other institutions. We are currently in the process of modernizing the facility with the goals of higher precision for routinely measured radio-nuclides, increased sample throughput, and the development of new measurement capabilities for the geoscience community.

  17. Identification of isotopically primitive interplanetary dust particles: A NanoSIMS isotopic imaging study

    SciTech Connect

    Floss, C; Stadermann, F J; Bradley, J P; Dai, Z R; Bajt, S; Graham, G; Lea, A S

    2005-09-02

    We have carried out a comprehensive survey of the isotopic compositions (H, B, C, N, O, S) of a suite of interplanetary dust particles (IDPs), including both cluster and individual particles. Isotopic imaging with the NanoSIMS shows the presence of numerous discrete hotspots that are strongly enriched in {sup 15}N, including the largest {sup 15}N enrichments ({approx}1300 {per_thousand}) observed in IDPs to date. A number of the IDPs also contain larger regions with more modest enrichments in {sup 15}N, leading to average bulk N isotopic compositions that are {sup 15}N-enriched in these IDPs. Although C isotopic compositions are normal in most of the IDPs, two {sup 15}N-rich N-hotspots have correlated {sup 13}C anomalies. CN{sup -}/C{sup -} ratios suggest that most of the {sup 15}N-rich hotspots are associated with relatively N-poor carbonaceous matter, although specific carriers have not been determined. H isotopic distributions are similar to those of N: D anomalies are present both as distinct very D-rich hotspots and as larger regions with more modest enrichments. Nevertheless, H and N isotopic anomalies are not directly correlated, consistent with results from previous studies. Oxygen isotopic imaging shows the presence of abundant presolar silicate grains in the IDPs. The O isotopic compositions of the grains are similar to those found in presolar oxide and silicate grains from primitive meteorites. Most of the silicate grains in the IDPs have isotopic ratios consistent with meteoritic Group 1 oxide grains, indicating origins in oxygen-rich red giant and asymptotic giant branch stars, but several presolar silicates exhibit the {sup 17}O and {sup 18}O enrichments of Group 4 oxide grains, whose origin is less well understood. Based on their N isotopic compositions, the IDPs studied here can be divided into two groups. One group is characterized as being ''isotopically primitive'' and consists of those IDPs that have anomalous bulk N isotopic compositions. These

  18. The Lithium Isotopic Signature of Hawaiian Basalts

    NASA Astrophysics Data System (ADS)

    Harrison, L.; Weis, D.; Hanano, D. W.

    2013-12-01

    Recycling of oceanic crust and sediment is a common mechanism to account for the presence of chemical heterogeneities observed in oceanic island basalts (OIBs). On Hawai';i, a mantle plume-sourced OIB with a high mass flux, sampling of deep mantle heterogeneities accounts for the presence of two unique geochemical and geographical trends called the Loa and Kea trends. The Loa trend overlaps the Pacific large low shear velocity province and is distinctly more enriched [1] than the Kea trend with average Pacific mantle compositions [2]. Because of the sizeable fractionation of lithium isotopes in low temperature environments, lithium serves as a tracer for the presence of recycled material in OIB sources, including Hawai'i. In this study, we analyzed 87 samples of Hawaiian basalt from the pre-shield, shield, post-shield, and rejuvenated volcanic stages and 10 samples of altered oceanic crust from ODP Site 843 for lithium isotopes using a multi-collector inductively coupled plasma mass spectrometer. Correlations of lithium isotopes with the radiogenic isotopes Pb, Hf, Nd, and Sr indicate lithium isotopes may be used to trace components in mantle plumes such as Hawai';i. The measured range of lithium isotopes for shield stage lavas is δ7Li = 1.8 - 5.7‰ and for post-shield lavas is δ7Li = 0.8 - 4.7‰. Pre-shield stage lavas (Lo'ihi volcano only) and rejuvenated lavas are the least and most homogeneous volcanic stages, respectively, in lithium isotopes. The Loa and Kea geochemical trends have different lithium isotopic signatures, with Loa trend shield volcanoes exhibiting lighter lithium isotopic signatures (δ7Li = 3.5‰ [N=43]) than Kea trend shield volcanoes (δ7Li = 4.0‰ [N=31]) [3]. Similarly, post-shield lavas have systematically lighter δ7Li than shield lavas. The presence of systematic differences in lithium isotopic signatures may indicate: 1) the sampling of distinct components in the deep source, to account for variations between Kea and Loa trend

  19. Magnesium isotopic compositions of the Mesoproterozoic dolostones: Implications for Mg isotopic systematics of marine carbonates

    NASA Astrophysics Data System (ADS)

    Huang, Kang-Jun; Shen, Bing; Lang, Xian-Guo; Tang, Wen-Bo; Peng, Yang; Ke, Shan; Kaufman, Alan J.; Ma, Hao-Ran; Li, Fang-Bing

    2015-09-01

    Available Mg isotope data indicate that dolostones of different ages have overlapping range of Mg isotopic composition (δ26Mg) and there is no systematic difference among different types of dolomites. To further explore the Mg isotopic systematics of dolomite formation, we measured Mg isotopic compositions of Mesoproterozoic dolostones from the Wumishan Formation in North China Block, because dolomite formation in Mesoproterozoic might have been fundamentally different from the younger counterparts. Based on petrographic observations, three texturally-different dolomite phases (dolomicrite, subhedral dolomite and anhedral dolomite) are recognized in the Wumishan dolostones. Nevertheless, these three types of dolomites have similar δ26Mg values, ranging from -1.35‰ to -1.72‰, which are indistinguishable from Neoproterozoic and Phanerozoic dolostones. To explain δ26Mg values of dolostones, we simulate the Mg isotopic system during dolomite formation by applying the one-dimensional Diffusion-Advection-Reaction (1D-DAR) model, assuming that the contemporaneous seawater is the Mg source of dolostone. The 1D-DAR modeling results indicate that the degree of dolomitization is controlled by sedimentation rate, seawater Mg concentration, temperature, and reaction rate of dolomite formation, whereas Mg isotopic composition of dolostone is not only dependent on these factors, but also affected by δ26Mg of seawater and isotope fractionation during dolomite formation. Moreover, the 1D-DAR model predicts that dolomite formation within sediments has limited range of variation in δ26Mg with respect to limestones. Furthermore, the modeling results demonstrate that dolostone is always isotopically heavier than Ca-carbonate precipitated from seawater, explaining the systematic isotopic difference between dolostones and limestones. Finally, we can infer from the 1D-DAR model that early-formed dolostone at shallower depth of sediments is always isotopically lighter than that

  20. Chemical stability of levoglucosan: an isotopic perspective

    NASA Astrophysics Data System (ADS)

    Sang, Xuefang; Gensch, Iulia; Schlag, Patrick; Wildt, Juergen; Laumer, Werner; Kammer, Beatrix; Tillmann, Ralf; Chitwan, Ojha; Heinichen, Gesa; Kiendler-scharr, Astrid

    2014-05-01

    Levoglucosan, used in receptor models as a specific tracer of biomass burning aerosols, has long been considered chemically stable in the atmosphere. Recent laboratory investigations found significant chemical degradation of levoglucosan when exposed to OH radicals (Hennigan et al., 2010). Stable carbon isotopic analyses, complementarily to concentration measurements, can provide additional evidence for physical and chemical processing in the atmosphere, since chemical processing causes changes in the relative abundance between heavy and light isotopes due to kinetic isotope effect (KIE). In this study, the chemical stability of levoglucosan was studied by exploring the isotopic fractionation of the reactant during the oxidation by OH. Mixed particles with levoglucosan and ammonium sulfate were generated in a continuous-stirred flow reactor and exposed to different levels of OH. Levoglucosan chemical degradation as function of OH exposure was derived from the decrease of levoglucosan/(NH4)2SO4 concentration ratios using aerosol mass spectrometry (AMS). Filter samples were collected for off-line isotopic analyses. Liquid extraction - Gas Chromatography - Isotope Ratio Mass Spectrometry (LE-GC-IRMS) was applied to measure stable carbon isotope ratios of levoglucosan. The observed d13C became more positive with increasing OH exposure, showing isotopic fractionations up to 3 ‰ at a reactant conversion of 45%. From the dependence of levoglucosan d13C on the OH exposure, a KIE of 1.00451 was derived, being within the range of predicted values for alkanes and alkenes with the same number of carbon atoms. With known source isotopic composition of levoglucosan in biomass burning aerosol (Sang et al., 2012), ambient measurements of levoglucosan d13C composition can therefore be used to determine the extent of chemical processing at the observation site. Reference: Hennigan, C. J., et al. 2010. Levoglucosan stability in biomass burning particles exposed to hydroxyl radicals

  1. Isotopic Compositions of Uranium Reference Materials

    NASA Astrophysics Data System (ADS)

    Jacobsen, B.; Borg, L. E.; Williams, R. W.; Brennecka, G.; Hutcheon, I. D.

    2009-12-01

    Uranium isotopic compositions of a variety of U standard materials were measured at Lawrence Livermore National Laboratory and are reported here. Both thermal ionization mass spectrometry (TIMS) and multi-collector inductively couple plasma mass spectrometry (MC-ICPMS) were used to determine ratios of the naturally occurring isotopes of U. Establishing an internally coherent set of isotopic values for a range of U standards is essential for inter-laboratory comparison of small differences in 238U/235U, as well as the minor isotopes of U. Differences of ~1.3‰ are now being observed in 238U/235U in natural samples, and may play an important role in understanding U geochemistry where tracing the origin of U is aided by U isotopic compositions. The 238U/235U ratios were measured with a TRITON TIMS using a mixed 233U-236U isotopic tracer to correct for instrument fractionation. This tracer was extremely pure and resulted in only very minor corrections on the measured 238U/235U ratios of ~0.03. The values obtained for 238U/235U are: IRMM184 = 137.698 ± 0.020 (n=15), SRM950a = 137.870 ± 0.018 (n=8), and CRM112a = 137.866 ± 0.030 (n=16). Uncertainties represent 2 s.d. of the population. Our measured value for IRMM184 is in near-perfect agreement with the certified value of 137.697 ± 0.042. However, the U isotopic compositions of SRM950a and CRM112a are not certified. Minor isotopes of U were determined with a Nu Plasma HR MC-ICPMS and mass bias was corrected by sample/standard bracketing to IRMM184, using its certified 238U/235U ratio. Thus, the isotopic compositions determined using both instruments are compatible. The values obtained for 234U/235U are: SRM950a = (7.437 ± 0.043)x10-3 (n=18), and CRM112a = (7.281 ± 0.050)x10-3 (n=16), both of which are in good agreement with published values. The value for 236U/235U in SRM950a was determined to be (8.48 ± 2.63)x10-6, whereas 236U was not detected in CRM112a. We are currently obtaining the U isotopic composition of

  2. A Cr Isotope Proxy For Ocean Deoxygenation

    NASA Astrophysics Data System (ADS)

    Holmden, C. E.; Scheiderich, K. D.; Amini, M.; Francois, R. H. G. M.; Bacconais, I.

    2015-12-01

    The concentration and distribution of Cr in the oceans is strongly controlled by its oxidation state. Cr(VI) (as soluble chromate) is the dominant oxidation state in oxygenated seawater. Chromate is typically greater than 70% of total dissolved Cr in the open ocean, consistent with thermodynamic predictions. However, lower than average chromate concentrations in coastal seas and oxygen minimum zones suggest that chromate is being removed in these settings by reduction to Cr(III), which favours particle reactive species. Cr is an element whose isotopes are fractionated by redox changes. Reduction of Cr(VI) causes light isotopes of Cr to be enriched in the product Cr(III). Accordingly, any local-scale increase in reductive Cr removal fluxes will cause the seawater Cr concentration to decrease and the δ53Cr value to increase. A recent study of Cr isotopes in the oceans1 supports this prediction. Cr isotopes show a range of δ53Cr values correlating inversely with Cr concentration. The fractionation factor deduced from this correlation is -0.80 ±0.03 ‰ (2s) on a global scale. The difference in solubility of oxidized and reduced Cr in seawater, and the isotopic fractionation between them, is the basis on which the Cr isotope proxy may be used for tracing ocean deoxygenation events in the geological past. More specifically, changes in the size of the chromate inventory of seawater, both locally and globally, should be traceable from reconstructions of seawater-derived Cr isotope variations in marine sedimentary successions. Geological records of Cr isotope changes in the oceans during past deoxygenation events may be used to gauge the impact of global warming on future deoxygenation of the oceans, particularly if proxy records of temperature and ocean pH are also reconstructed. However, study of the modern ocean Cr cycle is still in its early stages, and important knowledge gaps need to be filled going forward. In this talk, we present results of our seawater Cr

  3. Site-Specific Carbon Isotopes in Organics

    NASA Astrophysics Data System (ADS)

    Piasecki, A.; Eiler, J. M.

    2012-12-01

    Natural organic molecules exhibit a wide range of internal site-specific isotope variation (i.e., molecules with same isotopic substitution type but different site). Such variations are generally unconstrained by bulk isotopic measurements. If known, site-specific variations might constrain temperatures of equilibrium, mechanisms of formation or consumption reactions, and possibly other details. For example, lipids can exhibit carbon isotope differences of up to 30‰ between adjacent carbon sites as a result of fractionations arising during decarboxylation of pyruvate and other steps in lipid biosynthesis(1). We present a method for site-specific carbon isotope analysis of propane, based on high-resolution, multi-collector gas source mass spectrometry, using a novel prototype instrument - the Thermo MAT 253 Ultra. This machine has an inlet system and electron bombardment ion source resembling those in conventional stable isotope gas source mass spectrometers, and the energy filter, magnet, and detector array resembling those in multi-collector ICPMS and TIMS. The detector array has 7 detector positions, 6 of which are movable, and each of which can collect ions with either a faraday cup (read through amplifiers ranging from 107-1012 ohms) or an SEM. High mass resolving power (up to 27,000, MRP = M/dM definition) is achieved through a narrow entrance slit, adjustable from 250 to 5 μm. Such resolution can cleanly separate isobaric interferences between isotopologues of organic molecules having the same cardinal mass (e.g., 13CH3 and 12CH2D). We use this technology to analyze the isotopologues and fragments of propane, and use such data to solve for the site-specific carbon isotope fractionation. By measuring isotopologues of both the one-carbon (13CH3) and the two-carbon (13C12CH4) fragment ion, we can solve for both bulk δ13C and the difference in δ13C between the terminal and central carbon position. We tested this method by analyzing mixtures between natural

  4. Isotopically pure magnesium isotope-24 is prepared from magnesium-24 oxide

    NASA Technical Reports Server (NTRS)

    Chellew, N. R.; Schilb, J. D.; Steunenberg, R. K.

    1968-01-01

    Apparatus is used to prepare isotopically pure magnesium isotope-24, suitable for use in neutron scattering and polarization experiments. The apparatus permits thermal reduction of magnesium-24 oxide with aluminum and calcium oxide, and subsequent vaporization of the product metal in vacuum. It uses a resistance-heated furnace tube and cap assembly.

  5. Analytical techniques in biomedical stable isotope applications: (isotope ratio) mass spectrometry or infrared spectrometry?

    PubMed

    Stellaard, Frans; Elzinga, Henk

    2005-12-01

    An overview is presented of biomedical applications of stable isotopes in general, but mainly focused on the activities of the Center for Liver, Digestive and Metabolic Diseases of the University Medical Center Groningen. The aims of metabolic studies in the areas of glucose, fat, cholesterol and protein metabolism are briefly explained, as well as the principle of breath testing and the techniques to study body composition and energy expenditure. Much attention is paid to the analytical considerations based upon metabolite concentrations, sample size restrictions, the availability of stable isotope labelled substrates and dose requirements in relation to compound-specific isotope analysis. The instrumental advantages and limitations of the generally used techniques gas chromatography/reaction/isotope ratio mass spectrometry and gas chromatography/mass spectrometry are described as well as the novelties of the recently commercialised liquid chromatography/combustion/isotope ratio mass spectrometry. The present use and future perspective of infrared (IR) spectrometry for clinical and biomedical stable isotope applications are reviewed. In this respect, the analytical demands on IR spectrometry are discussed to enable replacement of isotope ratio mass spectrometry by IR spectrometry, in particular, for the purpose of compound-specific isotope ratio analysis in biological matrices. PMID:16543190

  6. Iron Isotopic Fractionation in Early Planetary Crusts

    NASA Astrophysics Data System (ADS)

    Wang, K.; Moynier, F.; Dauphas, N.; Barrat, J.; Day, J. M.; Sio, C.; Korotev, R. L.; Zeigler, R. A.

    2012-12-01

    Differentiated meteorites (achondrites) derive from planetary bodies that experienced variable degrees of melting and silicate-metal segregation. The oldest achondrites, such as eucrites, angrites, brachinites and the oligoclase-rich meteorites Graves Nunataks 06128/06129 (GRA 06128/9), were formed ~2-5 Ma after the first Solar System solids. They represent the oldest differentiated silicate samples known in the Solar System and the study of these samples provides insight on the origins and conditions of formation of the first planetary crusts. Here, we present new high-precision data for the Fe isotopic compositions of eucrites, angrites, brachinites and GRA 06128/9 and interpret these results in terms of magmatism during formation of these samples. We find that most eucrites and brachinites are not fractionated compared to undifferentiated chondritic meteorites (δ56Fe = 0.00±0.01, 2se), while the rare Stannern-trend eucrites are slightly enriched in the heavier isotopes of Fe. Angrites are also enriched in the heavier isotopes (δ56Fe = 0.12±0.01, 2se), similar to what is observed for terrestrial basalts, reflecting the relatively high oxidation states of the angrite parent body(ies). Contrastingly to the 'basaltic' achondrites, GRA 06128/9 are enriched in light isotopes of Fe (δ56Fe = -0.08±0.02, 2se). Evidence for light Fe isotope enrichments may be the consequence of the segregation of magma rich in sulphide (usually enriched in light isotopes of Fe compared to silicate and metal in undifferentiated meteorites). If correct, this result not only confirms that GRA 06128/9 represent products from <30% partial melting of an asteroidal body, prior to core formation, but also indicates complementary Fe isotope systematics between GRA 06128/9 and brachinites.

  7. Calcium isotopic composition of mantle peridotites

    NASA Astrophysics Data System (ADS)

    Huang, F.; Kang, J.; Zhang, Z.

    2015-12-01

    Ca isotopes are useful to decipher mantle evolution and the genetic relationship between the Earth and chondrites. It has been observed that Ca isotopes can be fractionated at high temperature [1-2]. However, Ca isotopic composition of the mantle peridotites and fractionation mechanism are still poorly constrained. Here, we report Ca isotope composition of 12 co-existing pyroxene pairs in 10 lherzolites, 1 harzburgite, and 1 wehrlite xenoliths collected from Hainan Island (South Eastern China). Ca isotope data were measured on a Triton-TIMS using the double spike method at the Guangzhou Institute of Geochemistry, CAS. The long-term external error is 0.12‰ (2SD) based on repeated analyses of NIST SRM 915a and geostandards. δ44Ca of clinopyroxenes except that from the wehrlite ranges from 0.85‰ to 1.14‰, while opx yields a wide range from 0.98‰ up to 2.16‰. Co-existing pyroxene pairs show large ∆44Caopx-cpx (defined as δ44Caopx-δ44Cacpx) ranging from 0 to 1.23‰, reflecting equilibrium fractionation controlled by variable Ca contents in the opx. Notably, clinopyroxene of wehrlite shows extremely high δ44Ca (3.22‰). δ44Ca of the bulk lherzolites and harzburgites range from 0.86‰ to 1.14‰. This can be explained by extracting melts with slightly light Ca isotopic compositions. Finally, the high δ44Ca of the wehrlite (3.22‰) may reflect metasomatism by melt which has preferentially lost light Ca isotopes due to chemical diffusion during upwelling through the melt channel. [1] Amini et al (2009) GGR 33; [2] Huang et al (2010) EPSL 292.

  8. Modeling nuclear volume isotope effects in crystals

    PubMed Central

    Schauble, Edwin A.

    2013-01-01

    Mass-independent isotope fractionations driven by differences in volumes and shapes of nuclei (the field shift effect) are known in several elements and are likely to be found in more. All-electron relativistic electronic structure calculations can predict this effect but at present are computationally intensive and limited to modeling small gas phase molecules and clusters. Density functional theory, using the projector augmented wave method (DFT-PAW), has advantages in greater speed and compatibility with a three-dimensional periodic boundary condition while preserving information about the effects of chemistry on electron densities within nuclei. These electron density variations determine the volume component of the field shift effect. In this study, DFT-PAW calculations are calibrated against all-electron, relativistic Dirac–Hartree–Fock, and coupled-cluster with single, double (triple) excitation methods for estimating nuclear volume isotope effects. DFT-PAW calculations accurately reproduce changes in electron densities within nuclei in typical molecules, when PAW datasets constructed with finite nuclei are used. Nuclear volume contributions to vapor–crystal isotope fractionation are calculated for elemental cadmium and mercury, showing good agreement with experiments. The nuclear-volume component of mercury and cadmium isotope fractionations between atomic vapor and montroydite (HgO), cinnabar (HgS), calomel (Hg2Cl2), monteponite (CdO), and the CdS polymorphs hawleyite and greenockite are calculated, indicating preferential incorporation of neutron-rich isotopes in more oxidized, ionically bonded phases. Finally, field shift energies are related to Mössbauer isomer shifts, and equilibrium mass-independent fractionations for several tin-bearing crystals are calculated from 119Sn spectra. Isomer shift data should simplify calculations of mass-independent isotope fractionations in other elements with Mössbauer isotopes, such as platinum and uranium

  9. The Cu isotopic composition of iron meteorites

    NASA Astrophysics Data System (ADS)

    Bishop, Matthew Cole; Moynier, Frederic; Weinstein, Charlotte; Fraboulet, Jean-Gabriel; Wang, Kun; Foriel, Julien

    2012-02-01

    High-precision Cu isotopic compositions have been measured for the metal phase of 29 iron meteorites from various groups and for four terrestrial standards. The data are reported as the δ65Cu permil deviation of the 65Cu/63Cu ratio relative to the NIST SRM 976 standard. Terrestrial mantle rocks have a very narrow range of variations and scatter around zero. In contrast, iron meteorites show δ65Cu approximately 2.3‰ variations. Different groups of iron meteorites have distinct δ65Cu values. Nonmagmatic IAB-IIICD iron meteorites have similar δ65Cu (0.03 ± 0.08 and 0.12 ± 0.10, respectively), close to terrestrial values (approximately 0). The other group of nonmagmatic irons, IIE, is isotopically distinct (-0.69 ± 0.15). IVB is the iron meteorite group with the strongest elemental depletion in Cu and samples in this group are enriched in the lighter isotope (δ65Cu down to -2.26‰). Evaporation should have produced an enrichment in 65Cu over 63Cu (δ65Cu >0) and can therefore be ruled out as a mechanism for volatile loss in IVB meteorites. In silicate-bearing iron meteorites, Δ17O correlates with δ65Cu. This correlation between nonmass-dependent and mass-dependent parameters suggests that the Cu isotopic composition of iron meteorites has not been modified by planetary differentiation to a large extent. Therefore, Cu isotopic ratios can be used to confirm genetic links. Cu isotopes thus confirm genetic relationships between groups of iron meteorites (e.g., IAB and IIICD; IIIE and IIIAB); and between iron meteorites and chondrites (e.g., IIE and H chondrites). Several genetic connections between iron meteorites groups are confirmed by Cu isotopes, (e.g., IAB and IIICD; IIIE and IIIAB); and between iron meteorites and chondrites (e.g., IIE and H chondrites).

  10. Modeling nuclear volume isotope effects in crystals.

    PubMed

    Schauble, Edwin A

    2013-10-29

    Mass-independent isotope fractionations driven by differences in volumes and shapes of nuclei (the field shift effect) are known in several elements and are likely to be found in more. All-electron relativistic electronic structure calculations can predict this effect but at present are computationally intensive and limited to modeling small gas phase molecules and clusters. Density functional theory, using the projector augmented wave method (DFT-PAW), has advantages in greater speed and compatibility with a three-dimensional periodic boundary condition while preserving information about the effects of chemistry on electron densities within nuclei. These electron density variations determine the volume component of the field shift effect. In this study, DFT-PAW calculations are calibrated against all-electron, relativistic Dirac-Hartree-Fock, and coupled-cluster with single, double (triple) excitation methods for estimating nuclear volume isotope effects. DFT-PAW calculations accurately reproduce changes in electron densities within nuclei in typical molecules, when PAW datasets constructed with finite nuclei are used. Nuclear volume contributions to vapor-crystal isotope fractionation are calculated for elemental cadmium and mercury, showing good agreement with experiments. The nuclear-volume component of mercury and cadmium isotope fractionations between atomic vapor and montroydite (HgO), cinnabar (HgS), calomel (Hg2Cl2), monteponite (CdO), and the CdS polymorphs hawleyite and greenockite are calculated, indicating preferential incorporation of neutron-rich isotopes in more oxidized, ionically bonded phases. Finally, field shift energies are related to Mössbauer isomer shifts, and equilibrium mass-independent fractionations for several tin-bearing crystals are calculated from (119)Sn spectra. Isomer shift data should simplify calculations of mass-independent isotope fractionations in other elements with Mössbauer isotopes, such as platinum and uranium. PMID

  11. Modeling nuclear volume isotope effects in crystals

    NASA Astrophysics Data System (ADS)

    Schauble, Edwin A.

    2013-10-01

    Mass-independent isotope fractionations driven by differences in volumes and shapes of nuclei (the field shift effect) are known in several elements and are likely to be found in more. All-electron relativistic electronic structure calculations can predict this effect but at present are computationally intensive and limited to modeling small gas phase molecules and clusters. Density functional theory, using the projector augmented wave method (DFT-PAW), has advantages in greater speed and compatibility with a three-dimensional periodic boundary condition while preserving information about the effects of chemistry on electron densities within nuclei. These electron density variations determine the volume component of the field shift effect. In this study, DFT-PAW calculations are calibrated against all-electron, relativistic Dirac-Hartree-Fock, and coupled-cluster with single, double (triple) excitation methods for estimating nuclear volume isotope effects. DFT-PAW calculations accurately reproduce changes in electron densities within nuclei in typical molecules, when PAW datasets constructed with finite nuclei are used. Nuclear volume contributions to vapor-crystal isotope fractionation are calculated for elemental cadmium and mercury, showing good agreement with experiments. The nuclear-volume component of mercury and cadmium isotope fractionations between atomic vapor and montroydite (HgO), cinnabar (HgS), calomel (Hg2Cl2), monteponite (CdO), and the CdS polymorphs hawleyite and greenockite are calculated, indicating preferential incorporation of neutron-rich isotopes in more oxidized, ionically bonded phases. Finally, field shift energies are related to Mössbauer isomer shifts, and equilibrium mass-independent fractionations for several tin-bearing crystals are calculated from 119Sn spectra. Isomer shift data should simplify calculations of mass-independent isotope fractionations in other elements with Mössbauer isotopes, such as platinum and uranium.

  12. Nuclear Volume Effects in Equilibrium Stable Isotope Fractionations of Hg, Tl and Pb Isotope Systems

    NASA Astrophysics Data System (ADS)

    Yang, S.; Liu, Y.

    2014-12-01

    Many evidences showed that heavy isotope systems could be significantly fractionated as the consequence of the nuclear volume effect (NVE) or so-called nuclear field shift effect. Here we investigate NVEs of Hg, Tl and Pb isotope systems by using quantum chemistry computational methods with careful evaluation on quantum relativistic effects via the Dirac's formalism of full-electron wavefunction. Our results generally agree with previous studies but with noticeable differences in many cases. With the unique NVE driving force, equilibrium 202Hg/198Hg and 205Tl/203Tl isotopes can be fractionated up to 3.94‰ and 2.78‰ at 0℃, respectively, showing potentially large equilibrium isotope fractionations can be expected for future studies of these two isotope systems. Moreover, the NVE causes large mass-independent fractionations (MIF) for odd-mass isotopes (e.g., ∆199NVHg and ∆201NVHg) and small MIFs for even-mass isotopes (e.g., ∆200NVHg). For Pb isotope system, NVEs induce isotope fractionations up to 1.62‰ (207Pb/206Pb) and 4.06‰ (208Pb/206Pb) at 0℃. However, contributions from classical mass-dependent driving force are small, about 0.1-0.5‰ for 207Pb/206Pb and 0.2-0.9‰ for 208Pb/206Pb. We find that Pb4+-bearing species can be significantly enriched heavy isotopes than Pb2+-bearing species. Comparing to Pb0, Pb2+-bearing species even enrich lighter Pb isotopes. A very strange and interesting thing is that the beta value of Pb2+-bearing species can be smaller than the unity (1.000). Similar thing has been found on Tl+-bearing species. This is an impossible and unexplained situation if only based on classical mass-dependent isotope fractionation theory (e.g., Bigeleisen-Mayer equation). The consequence is that the different direction of beta values of Pb2+-bearing species will let the Pb isotope fractionation even larger when they fractionate with Pb4+-bearing species. Moreover, NVEs also cause mass-independent fractionation (MIF) of odd 207Pb

  13. Isotopic inferences of ancient biochemistries - Carbon, sulfur, hydrogen, and nitrogen

    NASA Technical Reports Server (NTRS)

    Schidlowski, M.; Hayes, J. M.; Kaplan, I. R.

    1983-01-01

    In processes of biological incorporation and subsequent biochemical processing sizable isotope effects occur as a result of both thermodynamic and kinetic fractionations which take place during metabolic and biosynthetic reactions. In this chapter a review is provided of earlier work and recent studies on isotope fractionations in the biogeochemical cycles of carbon, sulfur, hydrogen, and nitrogen. Attention is given to the biochemistry of carbon isotope fractionation, carbon isotope fractionation in extant plants and microorganisms, isotope fractionation in the terrestrial carbon cycle, the effects of diagenesis and metamorphism on the isotopic composition of sedimentary carbon, the isotopic composition of sedimentary carbon through time, implications of the sedimentary carbon isotope record, the biochemistry of sulfur isotope fractionation, pathways of the biogeochemical cycle of nitrogen, and the D/H ratio in naturally occurring materials.

  14. LANL-IPF responses to isotopes workshop background information survey

    SciTech Connect

    Nortier, Francois Meiring

    2008-01-01

    Responses to the following are provided: (A) Which isotopes do you (company, agency, university, community) currently use in your activities or distribute (repackage) to end-users? (B) Describe generally what these isotopes are used for, i.e. the science or application. (C) Which isotope(s) do you anticipate may have significant future increase in demand. Identify the isotope(s), its priority, possible chemical form and for what purpose it would be used. (D) Are there other isotopes that you might use but are currently unavilable or not available in difficient quantities? If so, please identify this isotope, from whom have you tired to obtain it and for what prupose would it be used. (E) Do you have any specific issues with respect to the purity, availability, reliability of supply, etc. of isotopes at present?

  15. Isotope Ratios of Cellulose from Plants Having Different Photosynthetic Pathways

    PubMed Central

    Sternberg, Leonel O.; Deniro, Michael J.; Johnson, Hyrum B.

    1984-01-01

    Hydrogen and carbon isotope ratios of cellulose nitrate and oxygen isotope ratios of cellulose from C3, C4, and Crassulacean acid metabolism (CAM) plants were determined for plants growing within a small area in Val Verde County, Texas. Plants having CAM had distinctly higher deuterium/hydrogen (D/H) ratios than plants having C3 and C4 metabolism. When hydrogen isotope ratios are plotted against carbon isotope ratios, each photosynthetic mode separates into a distinct cluster of points. C4 plants had many D/H ratios similar to those of C3 plants, so that hydrogen isotope ratios cannot be used to distinguish between these two photosynthetic modes. Portulaca mundula, which may have a modified photosynthetic mode between C4 and CAM, had a hydrogen isotope ratio between those of the C4 and CAM plants. When oxygen isotope ratios are plotted against carbon isotope ratios, no distinct clustering of the C4 and CAM plants occurs. Thus, oxygen isotope ratios are not useful in distinguishing between these metabolic modes. A plot of hydrogen isotope ratios versus oxygen isotope ratios for this sample set shows considerable overlap between oxygen isotope ratios of the different photosynthetic modes without a concomitant overlap in the hydrogen isotope ratios of CAM and the other two photosynthetic modes. This observation is consistent with the hypothesis that higher D/H ratios in CAM plants relative to C3 and C4 plants are due to isotopic fractionations occurring during biochemical reactions. PMID:16663460

  16. Molybdenum Isotopic Composition of Iron Meteorites, Chondrites and Refractory Inclusions

    NASA Technical Reports Server (NTRS)

    Becker, H.; Walker, R. J.

    2003-01-01

    Recent Mo isotopic studies of meteorites reported evidence for differences in isotopic compositions for whole rocks of some primitive and differentiated meteorites relative to terrestrial materials. Enrichments of r- and p-process isotopes of up to 3-4 units (e unit = parts in 10(exp 4) over s-process dominated isotopes are the most prominent features. Certain types of presolar grains show large enrichments in s-process isotopes, however, it was concluded on grounds of mass balance that incomplete digestion of such grains cannot explain the enrichments of r- and p-process isotopes in whole rocks of primitive chondrites. If the reported variability in r- and p-process isotope enrichments reflects the true isotopic characteristics of the whole rocks, the implications are quite profound. It would suggest the presence of large scale Mo isotopic heterogeneity within the solar accretion disk with likely collateral effects for other elements. However, such effects were not found for Ru isotopes, nor for Zr isotopes. Another recent Mo isotopic study by multi collector ICP-MS could not confirm the reported deviations in Allende, Murchison or iron meteorites. Here, we present new results for the Mo isotopic composition of iron meteorites, chondrites and CAIs obtained by negative thermal ionization mass spectrometry (NTIMS). We discuss analytical aspects and the homogeneity of Mo isotopic compositions in solar system materials.

  17. Determining Clumped Isotope (Δ47) Signatures of CO2 During Ion-Molecule Isotopic Exchange Reactions

    NASA Astrophysics Data System (ADS)

    Sarna, J.; Priyadarshi, A.; Pourmorady, P.; Tripati, A.; Estaris, J.

    2015-12-01

    The abundance of multiply-substituted isotopologues such as 13C16O18O can be used to understand fundamental mechanisms that controls isotopic fractionation in chemical reactions. Knowledge of the energy-dependent ion-molecule isotopic exchange rate for 13C16O18O may also provide important insights into the CO2 ion-molecular exchange that occurs in the source of the mass spectrometer. It may offer an explanation for the recently observed nonlinearities associated with clumped isotope measurements. We designed a controlled set of laboratory experiments to investigate variations in the abundance of 13C16O18O associated with different ion-molecular isotopic exchange reactions. In our experiments, we characterize the effects of changing ionization energy, reaction time, CO2 amount, the presence of different compounds, and reaction chamber temperature on the clumped isotopic composition of CO2.

  18. Resolving the stellar sources of isotopically rare presolar silicate grains through Mg and Fe isotopic analyses

    SciTech Connect

    Nguyen, Ann N.; Messenger, Scott

    2014-04-01

    We conducted multi-element isotopic analyses of 11 presolar silicate grains from the Acfer 094 meteorite having unusual O isotopic compositions. Eight grains are {sup 18}O-rich, one is {sup 16}O-rich, and two are extremely {sup 17}O-rich. We constrained the grains' stellar sources by measuring their Si and Mg isotopic ratios, and also the {sup 54}Fe/{sup 56}Fe and {sup 57}Fe/{sup 56}Fe ratios for five grains. The Mg and Fe isotopic measurements were conducted after surrounding matrix grains were removed for more accurate ratios. Most of the {sup 18}O-rich silicates had anomalous Mg isotopic ratios, and their combined isotopic constraints are consistent with origins in low-mass Type II supernovae (SNe II) rather than high-metallicity stars. The isotopic ratios of the {sup 16}O-rich silicate are also consistent with an SN origin. Mixing small amounts of interior stellar material with the stellar envelope replicated all measured isotopic ratios except for {sup 29}Si/{sup 28}Si and {sup 54}Fe/{sup 56}Fe in some grains. The {sup 29}Si/{sup 28}Si ratios of all SN-derived grains are matched by doubling the {sup 29}Si yield in the Ne- and Si-burning zones. The {sup 54}Fe/{sup 56}Fe ratios of the grains imply elemental fractionation in the Si/S zone, or introduction of isotopically solar Fe by secondary processing. The two highly {sup 17}O-rich silicates exhibited significant {sup 25}Mg and/or {sup 26}Mg enrichments and their isotopic ratios are best explained by strong dilution of 1.15 M {sub ☉} CO nova matter. We estimate that ∼12% and 1% of presolar silicates have SN and nova origins, respectively, similar to presolar SiC and oxides. This implies that asymptotic giant branch stars are the dominant dust producers in the galaxy.

  19. Palladium Isotopic Evidence for Nucleosynthetic and Cosmogenic Isotope Anomalies in IVB Iron Meteorites

    NASA Astrophysics Data System (ADS)

    Mayer, Bernhard; Wittig, Nadine; Humayun, Munir; Leya, Ingo

    2015-08-01

    The origin of ubiquitous nucleosynthetic isotope anomalies in meteorites may represent spatial and/or temporal heterogeneity in the sources that supplied material to the nascent solar nebula, or enhancement by chemical processing. For elements beyond the Fe peak, deficits in s-process isotopes have been reported in some (e.g., Mo, Ru, W) but not all refractory elements studied (e.g., Os) that, among the iron meteorites, are most pronounced in IVB iron meteorites. Palladium is a non-refractory element in the same mass region as Mo and Ru. In this study, we report the first precise Pd isotopic abundances from IVB irons to test the mechanisms proposed for the origin of isotope anomalies. First, this study determined the existence of a cosmogenic neutron dosimeter from the reaction 103Rh(n, β-)104Pd in the form of excess 104Pd, correlated with excess 192Pt, in IVB irons. Second, all IVB irons show a deficit of the s-process only isotope 104Pd (\\varepsilon 104Pd = -0.48 ± 0.24), an excess of the r-only isotope 110Pd (\\varepsilon 110Pd = +0.46 ± 0.12), and no resolvable anomaly in the p-process 102Pd (\\varepsilon 102Pd = +1 ± 1). The magnitude of the Pd isotope anomaly is about half that predicted from a uniform depletion of the s-process yields from the correlated isotope anomalies of refractory Mo and Ru. The discrepancy is best understood as the result of nebular processing of the less refractory Pd, implying that all the observed nucleosynthetic anomalies in meteorites are likely to be isotopic relicts. The Mo-Ru-Pd isotope systematics do not support enhanced rates of the 22Ne(α,n)25Mg neutron source for the solar system s-process.

  20. Myths of Isotopic Reference Materials Busted

    NASA Astrophysics Data System (ADS)

    Coplen, T.

    2007-12-01

    During the past several years, the determination of the isotopic abundances of elements including H, Li, B, C, N, O, Mg, Si, S, Cl, Ca, Cr, Fe, Cu, Zn, Tl, and Se has substantially increased because of expanded use in hydrology, environmental studies, microbiology, forensic investigations, atmospheric investigations, oceanography, etc. Improvements in instrumentation enable increasingly precise isotope-amount-ratio measurements in these fields, but these improvements in precision commonly do not lead to improvements in accuracy because of the lack or improper use of isotopic reference materials. When properly used, these critically important materials enable any laboratory worldwide to measure the same homogeneous sample and report the same isotopic abundance within analytical uncertainty. For example, for stable isotopic analysis of gaseous hydrogen samples, the agreement among 36 laboratories worldwide before normalization to any hydrogen gas reference material was 11.8 per mill. After normalization to anchors (gaseous H isotopic reference materials) at each end of the delta H-2 scale, the agreement was 0.85 per mill, an improvement of more than an order of magnitude. Consistency of delta C-13 measurements often can be improved by nearly 50 percent by anchoring the delta C-13 scale with two isotopic reference materials differing substantially in C-13 mole fraction, namely NBS 19 calcite and L-SVEC lithium carbonate. Agreement of delta C-13 values of four expert laboratories analyzing USGS40 L- glutamic acid by CF-IRMS methods improved from 0.084 to 0.015 per mill with use of the two scale anchors (NBS 19 and L-SVEC). Solid oxygen isotopic reference materials (IAEA-600 caffeine, IAEA-601 and IAEA-602 benzoic acids, IAEA-NO-3, USGS32, USGS34, and USGS35 nitrates, NBS-127, IAEA-SO-5, and IAEA-SO-6 barium sulfates) are poorly calibrated. Calibrating these solids to the VSMOW-SLAP reference water scale has been very difficult because both the solids and reference