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.

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.

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.

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.

Biomedical research applications of electromagnetically separated enriched stable isotopes

NASA Astrophysics Data System (ADS)

Lambrecht, R. M.

The current and projected annual requirements through 1985 for stable isotopes enriched by electromagnetic separation methods were reviewed for applications in various types of biomedical research: (1) medical radiosiotope production, labeled compounds, and potential radio-pharmaceuticals; (2) nutrition, food science, and pharmacology: (3) metallobiochemistry and environmental toxicology; (4) nuclear magnetic resonance, electron paramagnetic resonance, and moessbauer spectroscopy in biochemical, biophysical, and biomedical research; and (5) miscellaneous advances in radioactive and nonradioactive tracer technology. Radioisotopes available from commercial sources or routinely used in clinical nuclear medicine were excluded. Current requirements for enriched stable isotopes in biomedical research are not being satisfied. Severe shortages exist for Mg 26, Ca 43, Zn 70, Se 76, Se 77, Se 78, Pd 102, Cd 111, Cd 113, and Os 190. Many interesting and potentially important investigations in biomedical research require small quantities of specific elements at high isotopic enrichments.

Isotope Separation in Concurrent Gas Centrifuges

NASA Astrophysics Data System (ADS)

Bogovalov, S. V.; Borman, V. D.

An analytical equation defining separative power of an optimized concurrent gas centrifuge is obtained for an arbitrary binary mixture of isotopes. In the case of the uranium isotopes the equation gives δU= 12.7(V/700 m/s)2(300 K/T)L, kg SWU/yr, where L and V are the length and linear velocity of the rotor of the gas centrifuge, T is the temperature. This formula well agrees with an empirical separative power of counter current gas centrifuges.

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.

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.

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.

Hydrogen isotope separation utilizing bulk getters

DOEpatents

Knize, R.J.; Cecchi, J.L.

1991-08-20

Tritium and deuterium are separated from a gaseous mixture thereof, derived from a nuclear fusion reactor or some other source, by providing a casing with a bulk getter therein for absorbing the gaseous mixture to produce an initial loading of the getter, partially desorbing the getter to produce a desorbed mixture which is tritium-enriched, pumping the desorbed mixture into a separate container, the remaining gaseous loading in the getter being deuterium-enriched, desorbing the getter to a substantially greater extent to produce a deuterium-enriched gaseous mixture, and removing the deuterium-enriched mixture into another container. The bulk getter may comprise a zirconium-aluminum alloy, or a zirconium-vanadium-iron alloy. The partial desorption may reduce the loading by approximately fifty percent. The basic procedure may be extended to produce a multistage isotope separator, including at least one additional bulk getter into which the tritium-enriched mixture is absorbed. The second getter is then partially desorbed to produce a desorbed mixture which is further tritium-enriched. The last-mentioned mixture is then removed from the container for the second getter, which is then desorbed to a substantially greater extent to produce a desorbed mixture which is deuterium-enriched. The last-mentioned mixture is then removed so that the cycle can be continued and repeated. The method of isotope separation is also applicable to other hydrogen isotopes, in that the method can be employed for separating either deuterium or tritium from normal hydrogen. 4 figures.

Hydrogen isotope separation utilizing bulk getters

DOEpatents

Knize, Randall J.; Cecchi, Joseph L.

1991-01-01

Tritium and deuterium are separated from a gaseous mixture thereof, derived from a nuclear fusion reactor or some other source, by providing a casing with a bulk getter therein for absorbing the gaseous mixture to produce an initial loading of the getter, partially desorbing the getter to produce a desorbed mixture which is tritium-enriched, pumping the desorbed mixture into a separate container, the remaining gaseous loading in the getter being deuterium-enriched, desorbing the getter to a substantially greater extent to produce a deuterium-enriched gaseous mixture, and removing the deuterium-enriched mixture into another container. The bulk getter may comprise a zirconium-aluminum alloy, or a zirconium-vanadium-iron alloy. The partial desorption may reduce the loading by approximately fifty percent. The basic procedure may be extended to produce a multistage isotope separator, including at least one additional bulk getter into which the tritium-enriched mixture is absorbed. The second getter is then partially desorbed to produce a desorbed mixture which is further tritium-enriched. The last-mentioned mixture is then removed from the container for the second getter, which is then desorbed to a substantially greater extent to produce a desorbed mixture which is deuterium-enriched. The last-mentioned mixture is then removed so that the cycle can be continued and repeated. The method of isotope separation is also applicable to other hydrogen isotopes, in that the method can be employed for separating either deuterium or tritium from normal hydrogen.

Hydrogen isotope separation utilizing bulk getters

DOEpatents

Knize, Randall J.; Cecchi, Joseph L.

1990-01-01

Tritium and deuterium are separated from a gaseous mixture thereof, derived from a nuclear fusion reactor or some other source, by providing a casing with a bulk getter therein for absorbing the gaseous mixture to produce an initial loading of the getter, partially desorbing the getter to produce a desorbed mixture which is tritium-enriched, pumping the desorbed mixture into a separate container, the remaining gaseous loading in the getter being deuterium-enriched, desorbing the getter to a substantially greater extent to produce a deuterium-enriched gaseous mixture, and removing the deuterium-enriched mixture into another container. The bulk getter may comprise a zirconium-aluminum alloy, or a zirconium-vanadium-iron alloy. The partial desorption may reduce the loading by approximately fifty percent. The basic procedure may be extended to produce a multistage isotope separator, including at least one additional bulk getter into which the tritium-enriched mixture is absorbed. The second getter is then partially desorbed to produce a desorbed mixture which is further tritium-enriched. The last-mentioned mixture is then removed from the container for the second getter, which is then desorbed to a substantially greater extent to produce a desorbed mixture which is deuterium-enriched. The last-mentioned mixture is then removed so that the cycle can be continued and repeated. The method of isotope separation is also applicable to other hydrogen isotopes, in that the method can be employed for separating either deuterium or tritium from normal hydrogen.

Isotope separation by photodissociation of Van der Waal's molecules

DOEpatents

Lee, Yuan T.

1977-01-01

A method of separating isotopes based on the dissociation of a Van der Waal's complex. A beam of molecules of a Van der Waal's complex containing, as one partner of the complex, a molecular species in which an element is present in a plurality of isotopes is subjected to radiation from a source tuned to a frequency which will selectively excite vibrational motion by a vibrational transition or through electronic transition of those complexed molecules of the molecular species which contain a desired isotope. Since the Van der Waal's binding energy is much smaller than the excitational energy of vibrational motion, the thus excited Van der Waal's complex dissociate into molecular components enriched in the desired isotope. The recoil velocity associated with vibrational to translational and rotational relaxation will send the separated molecules away from the beam whereupon the product enriched in the desired isotope can be separated from the constituents of the beam.

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.

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.

Apparatus for separating and recovering hydrogen isotopes

DOEpatents

Heung, Leung K.

1994-01-01

An apparatus for recovering hydrogen and separating its isotopes. The apparatus includes a housing bearing at least a fluid inlet and a fluid outlet. A baffle is disposed within the housing, attached thereto by a bracket. A hollow conduit is coiled about the baffle, in spaced relation to the baffle and the housing. The coiled conduit is at least partially filled with a hydride. The hydride can be heated to a high temperature and cooled to a low temperature quickly by circulating a heat transfer fluid in the housing. The spacing between the baffle and the housing maximizes the heat exchange rate between the fluid in the housing and the hydride in the conduit. The apparatus can be used to recover hydrogen isotopes (protium, deuterium and tritium) from gaseous mixtures, or to separate hydrogen isotopes from each other.

VELOCITY SELECTOR METHOD FOR THE SEPARATION OF ISOTOPES

DOEpatents

Britten, R.J.

1957-12-31

A velocity selector apparatus is described for separating and collecting an enriched fraction of the isotope of a particular element. The invention has the advantage over conventional mass spectrometers in that a magnetic field is not used, doing away with the attendant problems of magnetic field variation. The apparatus separates the isotopes by selectively accelerating the ionized constituents present in a beam of the polyisotopic substance that are of uniform kinetic energy, the acceleration being applied intermittently and at spaced points along the beam and in a direction normal to the direction of the propagation of the uniform energy beam whereby a transverse displacement of the isotopic constituents of different mass is obtained.

Laser-induced separation of hydrogen isotopes in the liquid phase

DOEpatents

Freund, Samuel M.; Maier, II, William B.; Beattie, Willard H.; Holland, Redus F.

1980-01-01

Hydrogen isotope separation is achieved by either (a) dissolving a hydrogen-bearing feedstock compound in a liquid solvent, or (b) liquefying a hydrogen-bearing feedstock compound, the liquid phase thus resulting being kept at a temperature at which spectral features of the feedstock relating to a particular hydrogen isotope are resolved, i.e., a clear-cut isotope shift is delineated, irradiating the liquid phase with monochromatic radiation of a wavelength which at least preferentially excites those molecules of the feedstock containing a first hydrogen isotope, inducing photochemical reaction in the excited molecules, and separating the reaction product containing the first isotope from the liquid phase.

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.

The ADvanced SEParation (ADSEP)

NASA Technical Reports Server (NTRS)

1998-01-01

The ADvanced SEParation (ADSEP) commercial payload is making use of major advances in separation technology: The Phase Partitioning Experiment (PPE); the Micorencapsulation experiment; and the Hemoglobin Separation Experiment (HSE). Using ADSEP, commercial researchers will attempt to determine the partition coefficients for model particles in a two-phase system. With this information, researchers can develop a higher resolution, more effective cell isolation procedure that can be used for many different types of research and for improved health care. The advanced separation technology is already being made available for use in ground-based laboratories.

Separation of isotopes by cyclical processes

DOEpatents

Hamrin, Jr., Charles E.; Weaver, Kenny

1976-11-02

Various isotopes of hydrogen are separated by a cyclic sorption process in which a gas stream containing the isotopes is periodically passed through a high pressure column containing a palladium sorbent. A portion of the product from the high pressure column is passed through a second column at lower pressure to act as a purge. Before the sorbent in the high pressure column becomes saturated, the sequence is reversed with the stream flowing through the former low-pressure column now at high pressure, and a portion of the product purging the former high pressure column now at low pressure. The sequence is continued in cyclic manner with the product being enriched in a particular isotope.

Validation of Electrochemically Modulated Separations Performed On-Line with MC-ICP-MS for Uranium and Plutonium Isotopic Analyses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liezers, Martin; Olsen, Khris B.; Mitroshkov, Alexandre V.

2010-08-11

The most time consuming process in uranium or plutonium isotopic analyses is performing the requisite chromatographic separation of the actinides. Filament preparation for thermal ionization (TIMS) adds further delays, but is generally accepted due to the unmatched performance in trace isotopic analyses. Advances in Multi-Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS) are beginning to rival the performance of TIMS. Methods, such as Electrochemically Modulated Separations (EMS) can efficiently pre-concentrate U or Pu quite selectively from small solution volumes in a matrix of 0.5 M nitric acid. When performed in-line with ICP-MS, the rapid analyte release from the electrode is fast,more » and large transient analyte signal enhancements of >100 fold can be achieved as compared to more conventional continuous nebulization of the original starting solution. This makes the approach ideal for very low level isotope ratio measurements. In this paper, some aspects of EMS performance are described. These include low level Pu isotope ratio behavior versus concentration by MC-ICP-MS and uranium rejection characteristics that are also important for reliable low level Pu isotope ratio determinations.« less

Uranium isotope separation from 1941 to the present

NASA Astrophysics Data System (ADS)

Maier-Komor, Peter

2010-02-01

Uranium isotope separation was the key development for the preparation of highly enriched isotopes in general and thus became the seed for target development and preparation for nuclear and applied physics. In 1941 (year of birth of the author) large-scale development for uranium isotope separation was started after the US authorities were warned that NAZI Germany had started its program for enrichment of uranium and might have confiscated all uranium and uranium mines in their sphere of influence. Within the framework of the Manhattan Projects the first electromagnetic mass separators (Calutrons) were installed and further developed for high throughput. The military aim of the Navy Department was to develop nuclear propulsion for submarines with practically unlimited range. Parallel to this the army worked on the development of the atomic bomb. Also in 1941 plutonium was discovered and the production of 239Pu was included into the atomic bomb program. 235U enrichment starting with natural uranium was performed in two steps with different techniques of mass separation in Oak Ridge. The first step was gas diffusion which was limited to low enrichment. The second step for high enrichment was performed with electromagnetic mass spectrometers (Calutrons). The theory for the much more effective enrichment with centrifugal separation was developed also during the Second World War, but technical problems e.g. development of high speed ball and needle bearings could not be solved before the end of the war. Spying accelerated the development of uranium separation in the Soviet Union, but also later in China, India, Pakistan, Iran and Iraq. In this paper, the physical and chemical procedures are outlined which lead to the success of the project. Some security aspects and Non-Proliferation measures are discussed.

Mathematical Model of Nonstationary Separation Processes Proceeding in the Cascade of Gas Centrifuges in the Process of Separation of Multicomponent Isotope Mixtures

NASA Astrophysics Data System (ADS)

Orlov, A. A.; Ushakov, A. A.; Sovach, V. P.

2017-03-01

We have developed and realized on software a mathematical model of the nonstationary separation processes proceeding in the cascades of gas centrifuges in the process of separation of multicomponent isotope mixtures. With the use of this model the parameters of the separation process of germanium isotopes have been calculated. It has been shown that the model adequately describes the nonstationary processes in the cascade and is suitable for calculating their parameters in the process of separation of multicomponent isotope mixtures.

Laser-assisted isotope separation of tritium

DOEpatents

Herman, Irving P.; Marling, Jack B.

1983-01-01

Methods for laser-assisted isotope separation of tritium, using infrared multiple photon dissociation of tritium-bearing products in the gas phase. One such process involves the steps of (1) catalytic exchange of a deuterium-bearing molecule XYD with tritiated water DTO from sources such as a heavy water fission reactor, to produce the tritium-bearing working molecules XYT and (2) photoselective dissociation of XYT to form a tritium-rich product. By an analogous procedure, tritium is separated from tritium-bearing materials that contain predominately hydrogen such as a light water coolant from fission or fusion reactors.

Resonance ionization laser ion sources for on-line isotope separators (invited).

PubMed

Marsh, B A

2014-02-01

A Resonance Ionization Laser Ion Source (RILIS) is today considered an essential component of the majority of Isotope Separator On Line (ISOL) facilities; there are seven laser ion sources currently operational at ISOL facilities worldwide and several more are under development. The ionization mechanism is a highly element selective multi-step resonance photo-absorption process that requires a specifically tailored laser configuration for each chemical element. For some isotopes, isomer selective ionization may even be achieved by exploiting the differences in hyperfine structures of an atomic transition for different nuclear spin states. For many radioactive ion beam experiments, laser resonance ionization is the only means of achieving an acceptable level of beam purity without compromising isotope yield. Furthermore, by performing element selection at the location of the ion source, the propagation of unwanted radioactivity downstream of the target assembly is reduced. Whilst advances in laser technology have improved the performance and reliability of laser ion sources and broadened the range of suitable commercially available laser systems, many recent developments have focused rather on the laser/atom interaction region in the quest for increased selectivity and/or improved spectral resolution. Much of the progress in this area has been achieved by decoupling the laser ionization from competing ionization processes through the use of a laser/atom interaction region that is physically separated from the target chamber. A new application of gas catcher laser ion source technology promises to expand the capabilities of projectile fragmentation facilities through the conversion of otherwise discarded reaction fragments into high-purity low-energy ion beams. A summary of recent RILIS developments and the current status of laser ion sources worldwide is presented.

Separative analyses of a chromatographic column packed with a core-shell adsorbent for lithium isotope separation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sugiyama, T.; Sugura, K.; Enokida, Y.

2015-03-15

Lithium-6 is used as a blanket material for sufficient tritium production in DT fueled fusion reactors. A core-shell type adsorbent was proposed for lithium isotope separation by chromatography. The mass transfer model in a chromatographic column consisted of 4 steps, such as convection and dispersion in the column, transfer through liquid films, intra-particle diffusion and and adsorption or desorption at the local adsorption sites. A model was developed and concentration profiles and time variation in the column were numerically simulated. It became clear that core-shell type adsorbents with thin porous shell were saturated rapidly relatively to fully porous one andmore » established a sharp edge of adsorption band. This is very important feature because lithium isotope separation requires long-distance development of adsorption band. The values of HETP (Height Equivalent of a Theoretical Plate) for core-shell adsorbent packed column were estimated by statistical moments of the step response curve. The value of HETP decreased with the thickness of the porous shell. A core-shell type adsorbent is, then, useful for lithium isotope separation. (authors)« less

Laser isotope separation by multiple photon absorption

DOEpatents

Robinson, C.P.; Rockwood, S.D.; Jensen, R.J.; Lyman, J.L.; Aldridge, J.P. III.

1987-04-07

Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, is the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO[sub 2] laser light may be used to highly enrich [sup 34]S in natural SF[sub 6] and [sup 11]B in natural BCl[sub 3]. 8 figs.

Laser isotope separation by multiple photon absorption

DOEpatents

Robinson, C. Paul; Rockwood, Stephen D.; Jensen, Reed J.; Lyman, John L.; Aldridge, III, Jack P.

1987-01-01

Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, is the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO.sub.2 laser light may be used to highly enrich .sup.34 S in natural SF.sub.6 and .sup.11 B in natural BCl.sub.3.

Laser isotope separation by multiple photon absorption

DOEpatents

Robinson, C. Paul; Rockwood, Stephen D.; Jensen, Reed J.; Lyman, John L.; Aldridge, III, Jack P.

1977-01-01

Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, in the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO.sub.2 laser light may be used to highly enrich .sup.34 S in natural SF.sub.6 and .sup.11 B in natural BCl.sub.3.

Separation efficiency of the MASHA facility for short-lived mercury isotopes

NASA Astrophysics Data System (ADS)

Rodin, A. M.; Belozerov, A. V.; Chernysheva, E. V.; Dmitriev, S. N.; Gulyaev, A. V.; Gulyaeva, A. V.; Itkis, M. G.; Kliman, J.; Kondratiev, N. A.; Krupa, L.; Novoselov, A. S.; Oganessian, Yu. Ts.; Podshibyakin, A. V.; Salamatin, V. S.; Siváček, I.; Stepantsov, S. V.; Vanin, D. V.; Vedeneev, V. Yu.; Yukhimchuk, S. A.; Granja, C.; Pospisil, S.

2014-06-01

The mass-separator MASHA built to identify Super Heavy Elements by their mass-to-charge ratios is described. The results of the off- and on-line measurements of its separation efficiency are presented. In the former case four calibrated leaks of noble gases were used. In the latter the efficiency was measured via 284 MeV Ar beam and with using the hot catcher. The ECR ion source was used in both cases. The -radioactive isotopes of mercury produced in the complete fusion reaction Ar+SmHg+xn were detected at the mass-separator focal plane. The half-lives and the separation efficiency for the short-lived mercury isotopes were measured. Potentialities of the MEDIPIX detector system have been demonstrated for future use at the mass-separator MASHA.

Liquid-phase thermal diffusion isotope separation apparatus and method having tapered column

DOEpatents

Rutherford, William M.

1988-05-24

A thermal diffusion counterflow method and apparatus for separating isotopes in solution in which the solution is confined in a long, narrow, vertical slit which tapers from bottom to top. The variation in the width of the slit permits maintenance of a stable concentration distribution with relatively long columns, thus permitting isotopic separation superior to that obtainable in the prior art.

Liquid-phase thermal diffusion isotope separation apparatus and method having tapered column

DOEpatents

Rutherford, W.M.

1985-12-04

A thermal diffusion counterflow method and apparatus for separating isotopes in solution in which the solution is confined in a long, narrow, vertical slit which tapers from bottom to top. The variation in the width of the slit permits maintenance of a stable concentration distribution with relatively long columns, thus permitting isotopic separation superior to that obtained in the prior art.

Influence of liquid structure on diffusive isotope separation in molten silicates and aqueous solutions

NASA Astrophysics Data System (ADS)

Watkins, James M.; DePaolo, Donald J.; Ryerson, Frederick J.; Peterson, Brook T.

2011-06-01

Molecular diffusion in natural volcanic liquids discriminates between isotopes of major ions (e.g., Fe, Mg, Ca, and Li). Although isotope separation by diffusion is expected on theoretical grounds, the dependence on mass is highly variable for different elements and in different media. Silicate liquid diffusion experiments using simple liquid compositions were carried out to further probe the compositional dependence of diffusive isotopic discrimination and its relationship to liquid structure. Two diffusion couples consisting of the mineral constituents anorthite (CaAl 2Si 2O 8; denoted AN), albite (NaAlSi 3O 8; denoted AB), and diopside (CaMgSi 2O 6; denoted DI) were held at 1450 °C for 2 h and then quenched to ambient pressure and temperature. Major-element as well as Ca and Mg isotope profiles were measured on the recovered quenched glasses. In both experiments, Ca diffuses rapidly with respect to Si. In the AB-AN experiment, D Ca/ D Si ≈ 20 and the efficiency of isotope separation for Ca is much greater than in natural liquid experiments where D Ca/ D Si ≈ 1. In the AB-DI experiment, D Ca/ D Si ≈ 6 and the efficiency of isotope separation is between that of the natural liquid experiments and the AB-AN experiment. In the AB-DI experiment, D Mg/ D Si ≈ 1 and the efficiency of isotope separation for Mg is smaller than it is for Ca yet similar to that observed for Mg in natural liquids. The results from the experiments reported here, in combination with results from natural volcanic liquids, show clearly that the efficiency of diffusive separation of Ca isotopes is systematically related to the solvent-normalized diffusivity - the ratio of the diffusivity of the cation ( D Ca) to the diffusivity of silicon ( D Si). The results on Ca isotopes are consistent with available data on Fe, Li, and Mg isotopes in silicate liquids, when considered in terms of the parameter D cation/ D Si. Cations diffusing in aqueous solutions display a similar relationship

Investigation of the Photochemical Method for Uranium Isotope Separation

DOE R&D Accomplishments Database

Urey, H. C.

1943-07-10

To find a process for successful photochemical separation of isotopes several conditions have to be fulfilled. First, the different isotopes have to show some differences in the spectrum. Secondly, and equally important, this difference must be capable of being exploited in a photochemical process. Parts A and B outline the physical and chemical conditions, and the extent to which one might expect to find them fulfilled. Part C deals with the applicability of the process.

A novel procedure for Rubidium separation and its isotope measurements on geological samples by MC-ICP-MS

NASA Astrophysics Data System (ADS)

Ma, J.; Zhang, Z.; Wei, G.; Zhang, L.

2017-12-01

A method including a novel column Rb separation procedure and high-precision Rb isotope measurement in geological materials by using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) in standard-sample-bracketing (SSB) mode has been developed. Sr-Spec resin was employed, in which the distribution coefficients for Rb, K, Ba and Sr are different in nitric acid, to sequentially separate them from the matrix. The dissolved samples were loaded on the column in 3 M HNO3, the main matrix such as Al, Ca, Fe, Mg, Mn and Na were removed by rinsing with 4.5 mL HNO3, Rb and K were then sequentially eluted by 3 M HNO3 in different volumes. After that, Ba was eluted by 8 M HNO3, and Sr was finally eluted by Milli-Q water. This enable us to collect the pure Rb, K, Ba and Sr one by one with recovery close to 100% for their isotopic compositions measurement on MC-ICP-MS. We here focus on Rb isotope measurement. The measurement using MC-ICP-MS yielded an internal precision for δ87Rb of < ± 0.03‰ (2SE), and the external precision was generally better than ± 0.06‰ (2SD) based on the long-term results of the Rb standard solutions NIST SRM 984. A series of geological rock standards, were analyzed using this method, and the results indicate significant Rb isotope differences in different geologic materials. This will provide a powerful tool to investigate Rb isotope fractionation during geological processes.Based on this method, Rb isotope compositions from a basaltic weathering profile were carried out. The data show the lighter Rb (85Rb) isotope is preferentially leached from the weathering profile and remains heavy Rb isotope (87Rb) in the weathered residues during the incipient weathering stage. From the moderate to advanced weathering stage, the significant variations of Rb isotope were observed and multiple factors, such as leaching, adsorption, desorption, and precipitation, should play important role in fractionating Rb isotope.

Separation of the isotopes of boron by chemical exchange reactions

DOEpatents

McCandless, F.P.; Herbst, R.S.

1995-05-30

The isotopes of boron, {sup 10}B and {sup 11}B, are separated by means of a gas-liquid chemical exchange reaction involving the isotopic equilibrium between gaseous BF{sub 3} and a liquid BF{sub 3} donor molecular addition complex formed between BF{sub 3} gas and a donor chosen from the group consisting of: nitromethane, acetone, methyl isobutyl ketone, or diisobutyl ketone. 1 Fig.

Separation of the isotopes of boron by chemical exchange reactions

DOEpatents

McCandless, Frank P.; Herbst, Ronald S.

1995-01-01

The isotopes of boron, .sup.10 B and .sup.11 B, are separated by means of a gas-liquid chemical exchange reaction involving the isotopic equilibrium between gaseous BF.sub.3 and a liquid BF.sub.3 . donor molecular addition complex formed between BF.sub.3 gas and a donor chosen from the group consisting of: nitromethane, acetone, methyl isobutyl ketone, or diisobutyl ketone.

Experimental equipment for an advanced ISOL facility[Isotope Separation On-Line Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baktash, C.; Lee, I.Y.; Rehm, K.E.

This report summarizes the proceedings and recommendations of the Workshop on the Experimental Equipment for an Advanced ISOL Facility which was held at Lawrence Berkeley National Laboratory on July 22--25, 1998. The purpose of this workshop was to discuss the performance requirements, manpower and cost estimates, as well as a schedule of the experimental equipment needed to fully exploit the new physics which can be studied at an advanced ISOL facility. An overview of the new physics opportunities that would be provided by such a facility has been presented in the White Paper that was issued following the Columbus Meeting.more » The reactions and experimental techniques discussed in the Columbus White Paper served as a guideline for the formulation of the detector needs at the Berkeley Workshop. As outlined a new ISOL facility with intense, high-quality beams of radioactive nuclei would provide exciting new research opportunities in the areas of: the nature of nucleonic matter; the origin of the elements; and tests of the Standard Model. After an introductory section, the following equipment is discussed: gamma-ray detectors; recoil separators; magnetic spectrographs; particle detectors; targets; and apparatus using non-accelerated beams.« less

Separation of uranium isotopes by chemical exchange

DOEpatents

Ogle, P.R. Jr.

1974-02-26

A chemical exchange method is provided for separating /sup 235/U from / sup 238/U comprising contacting a first phase containing UF/sub 6/ with a second phase containing a compound selected from the group consisting of NOUF/sub 6/, NOUF/sub 7/, and NO/sub 2/UF/sub 7/ until the U Fsub 6/ in the first phase becomes enriched in the /sup 235/U isotope. (Official Gazette)

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.

Separation of copper, iron, and zinc from complex aqueous solutions for isotopic measurement

USGS Publications Warehouse

Borrok, D.M.; Wanty, R.B.; Ridley, W.I.; Wolf, R.; Lamothe, P.J.; Adams, M.

2007-01-01

The measurement of Cu, Fe, and Zn isotopes in natural samples may provide valuable information about biogeochemical processes in the environment. However, the widespread application of stable Cu, Fe, and Zn isotope chemistry to natural water systems remains limited by our ability to efficiently separate these trace elements from the greater concentrations of matrix elements. In this study, we present a new method for the isolation of Cu, Fe, and Zn from complex aqueous solutions using a single anion-exchange column with hydrochloric acid media. Using this method we are able to quantitatively separate Cu, Fe, and Zn from each other and from matrix elements in a single column elution. Elution of the elements of interest, as well as all other elements, through the anion-exchange column is a function of the speciation of each element in the various concentrations of HCl. We highlight the column chemistry by comparing our observations with published studies that have investigated the speciation of Cu, Fe, and Zn in chloride solutions. The functionality of the column procedure was tested by measuring Cu, Fe, and Zn isotopes in a variety of stream water samples impacted by acid mine drainage. The accuracy and precision of Zn isotopic measurements was tested by doping Zn-free stream water with the Zn isotopic standard. The reproducibility of the entire column separation process and the overall precision of the isotopic measurements were also evaluated. The isotopic results demonstrate that the Cu, Fe, and Zn column separates from the tested stream waters are of sufficient purity to be analyzed directly using a multicollector inductively coupled plasma mass spectrometer (MC-ICP-MS), and that the measurements are fully-reproducible, accurate, and precise. Although limited in scope, these isotopic measurements reveal significant variations in ??65Cu (- 1.41 to + 0.30???), ??56Fe (- 0.56 to + 0.34???), and ??66Zn (0.31 to 0.49???) among samples collected from different

10 CFR Appendix N to Part 110 - Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's...

Code of Federal Regulations, 2014 CFR

2014-01-01

... 10 Energy 2 2014-01-01 2014-01-01 false Illustrative List of Lithium Isotope Separation Facilities... Appendix N to Part 110—Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's Export Licensing Authority a. Facilities or plants for the separation of lithium isotopes. b...

10 CFR Appendix N to Part 110 - Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's...

Code of Federal Regulations, 2012 CFR

2012-01-01

... 10 Energy 2 2012-01-01 2012-01-01 false Illustrative List of Lithium Isotope Separation Facilities... Appendix N to Part 110—Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's Export Licensing Authority a. Facilities or plants for the separation of lithium isotopes. b...

10 CFR Appendix N to Part 110 - Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's...

Code of Federal Regulations, 2013 CFR

2013-01-01

... 10 Energy 2 2013-01-01 2013-01-01 false Illustrative List of Lithium Isotope Separation Facilities... Appendix N to Part 110—Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's Export Licensing Authority a. Facilities or plants for the separation of lithium isotopes. b...

10 CFR Appendix N to Part 110 - Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's...

Code of Federal Regulations, 2011 CFR

2011-01-01

... 10 Energy 2 2011-01-01 2011-01-01 false Illustrative List of Lithium Isotope Separation Facilities... Appendix N to Part 110—Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's Export Licensing Authority a. Facilities or plants for the separation of lithium isotopes. b...

10 CFR Appendix N to Part 110 - Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's...

Code of Federal Regulations, 2010 CFR

2010-01-01

... 10 Energy 2 2010-01-01 2010-01-01 false Illustrative List of Lithium Isotope Separation Facilities... Appendix N to Part 110—Illustrative List of Lithium Isotope Separation Facilities, Plants and Equipment Under NRC's Export Licensing Authority a. Facilities or plants for the separation of lithium isotopes. b...

Recent advances in microparticle continuous separation.

PubMed

Kersaudy-Kerhoas, M; Dhariwal, R; Desmulliez, M P Y

2008-03-01

Recent advances in microparticle separation in continuous flow are presented. It is intended for scientists in the field of separation science in biology, chemistry and microsystems engineering. Recent techniques of micron-sized particle separation within microsystems are described with emphasis on five different categories: optical, magnetic, fluidic-only, electrical and minor separation methods. Examples from the growing literature are explained with insights on separation efficiency and microengineering challenges. Current applications of the techniques are discussed.

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.

CONTROL SYSTEM FOR ISOTOPE SEPARATING APPARATUS

DOEpatents

Barnes, S.W.

1960-01-26

A method is described for controlling the position of the ion beams in a calutron used for isotope separation. The U/sup 238/ beams is centered over the U/sup 235/ receiving pocket, the operator monitoring the beam until a maximum reading is achieved on the meter connected to that pocket. Then both beams are simultaneously shifted by a preselected amount to move the U/sup 235/ beam over the U/sup 235/ pocket. A slotted door is placed over the entrance to that pocket during the U/sup 238/ beam centering to reduce the contamination to the pocket, while allowing enough beam to pass for monitoring purposes.

Methods for separating medical isotopes using ionic liquids

DOEpatents

Luo, Huimin; Boll, Rose Ann; Bell, Jason Richard; Dai, Sheng

2014-10-21

A method for extracting a radioisotope from an aqueous solution, the method comprising: a) intimately mixing a non-chelating ionic liquid with the aqueous solution to transfer at least a portion of said radioisotope to said non-chelating ionic liquid; and b) separating the non-chelating ionic liquid from the aqueous solution. In preferred embodiments, the method achieves an extraction efficiency of at least 80%, or a separation factor of at least 1.times.10.sup.4 when more than one radioisotope is included in the aqueous solution. In particular embodiments, the method is applied to the separation of medical isotopes pairs, such as Th from Ac (Th-229/Ac-225, Ac-227/Th-227), or Ra from Ac (Ac-225 and Ra-225, Ac-227 and Ra-223), or Ra from Th (Th-227 and Ra-223, Th-229 and Ra-225).

Stable Isotope Quantitative N-Glycan Analysis by Liquid Separation Techniques and Mass Spectrometry.

PubMed

Mittermayr, Stefan; Albrecht, Simone; Váradi, Csaba; Millán-Martín, Silvia; Bones, Jonathan

2017-01-01

Liquid phase separation analysis and subsequent quantitation remains a challenging task for protein-derived oligosaccharides due to their inherent structural complexity and diversity. Incomplete resolution or co-detection of multiple glycan species complicates peak area-based quantitation and associated statistical analysis when optical detection methods are used. The approach outlined herein describes the utilization of stable isotope variants of commonly used fluorescent tags that allow for mass-based glycan identification and relative quantitation following separation by liquid chromatography (LC) or capillary electrophoresis (CE). Comparability assessment of glycoprotein-derived oligosaccharides is performed by derivatization with commercially available isotope variants of 2-aminobenzoic acid or aniline and analysis by LC- and CE-mass spectrometry. Quantitative information is attained from the extracted ion chromatogram/electropherogram ratios generated from the light and heavy isotope clusters.

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.

Hydrogen isotope separation using molecular sieve of synthetic zeolite 3A

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kotoh, K.; Kimura, K.; Nakamura, Y.

2008-07-15

It is known that hydrogen isotope molecules can be adsorbed easily onto synthetic zeolite 4A, 5A, and 13X at the liquid-nitrogen temperature of 77.4 K. We show here that hydrogen and deuterium are not adsorptive onto zeolite 3A at the same temperature. This phenomenon is explained by assuming the molecular sieve function in zeolite-3A-crystalline lattice structure. From a series of pseudo-isobaric experiments, it is also shown that the sieving phenomenon appears in a range above 77.4 K. This behavior is interpreted as resulting on the dependence of sieve's mesh size on temperature, where the sieving effect is considered to appearmore » at a certain temperature. In this interpretation, an isotopic difference between hydrogen and deuterium is suggested to exist in the sieving effect appearance temperatures. This is endorsed in the result of pseudo-isobaric experiments. This temperature deference is very significant because that indicates the possibility of an effective method of hydrogen isotope separation. This possibility is verified through an experimental series of adsorption-desorption with a mixture of H{sub 2} and D{sub 2}, where the gas samples adsorbed through the sieve operated at intentionally selected temperatures are isolated and then analyzed. The result demonstrates remarkable values of isotope separation factor. (authors)« less

Stormflow-hydrograph separation based on isotopes: the thrill is gone--what's next?

USGS Publications Warehouse

Burns, Douglas A.

2002-01-01

Beginning in the 1970s, the promise of a new method for separatingstormflow hydrographs using18O,2H, and3Hprovedanirresistibletemptation, and was a vast improvement over graphical separationand solute tracer methods that were prevalent at the time. Eventu-ally, hydrologists realized that this new method entailed a plethoraof assumptions about temporal and spatial homogeneity of isotopiccomposition (many of which were commonly violated). Nevertheless,hydrologists forged ahead with dozens of isotope-based hydrograph-separation studies that were published in the 1970s and 1980s.Hortonian overland flow was presumed dead. By the late 1980s,the new isotope-based hydrograph separation technique had movedinto adolescence, accompanied by typical adolescent problems suchas confusion and a search for identity. As experienced hydrologistscontinued to use the isotope technique to study stormflow hydrol-ogy in forested catchments in humid climates, their younger peersfollowed obligingly—again and again. Was Hortonian overland flowreally dead and forgotten, though? What about catchments in whichpeople live and work? And what about catchments in dry climatesand the tropics? How useful were study results when several of theassumptions about the homogeneity of source waters were commonlyviolated? What if two components could not explain the variation ofisotopic composition measured in the stream during stormflow? Andwhat about uncertainty? As with many new tools, once the initialshine wore off, the limitations of the method became a concern—oneof which was that isotope-based hydrograph separations alone couldnot reveal much about the flow paths by which water arrives at astream channel during storms.

A Mass Spectrometry Study of Isotope Separation in the Laser Plume

NASA Astrophysics Data System (ADS)

Suen, Timothy Wu

Accurate quantification of isotope ratios is critical for both preventing the development of illicit weapons programs in nuclear safeguards and identifying the source of smuggled material in nuclear forensics. While isotope analysis has traditionally been performed by mass spectrometry, the need for in situ measurements has prompted the development of optical techniques, such as laser-induced breakdown spectroscopy (LIBS) and laser ablation molecular isotopic spectrometry (LAMIS). These optical measurements rely on laser ablation for direct solid sampling, but several past studies have suggested that the distribution of isotopes in the ablation plume is not uniform. This study seeks to characterize isotope separation in the laser plume through the use of orthogonal-acceleration time-of-flight mass spectrometry. A silver foil was ablated with a Nd:YAG at 355 nm at an energy of 50 muJ with a spot size of 71 mum, for a fluence of 1.3 J/cm2 and an irradiance of 250 MW/cm2. Flat-plate repellers were used to sample the plume, and a temporal profile of the ions was obtained by varying the time delay on the high-voltage pulse. A spatial profile along the axis of the plume was generated by changing the position of the sample, which yielded snapshots of the isotopic composition with time. In addition, the reflectron time-of-flight system was used as an energy filter in conjunction with the repellers to sample slices of the laser plasma orthogonal to the plume axis. Mass spectrometry of the plume revealed a fast ion distribution and a slow ion distribution. Measurements taken across the entire plume showed the fast 109Ag ions slightly ahead in both space and time, causing the 107Ag fraction to drop to 0.34 at 3 mus, 4 mm from the sample surface. Although measurements centered on the near side of the plume did not show isotope separation, the slow ions on the far side of the plume included much more 109Ag than 107Ag. In addition to examining the isotope content of the ablation

Preparative separation of underivatized amino acids for compound-specific stable isotope analysis and radiocarbon dating of hydrolyzed bone collagen.

PubMed

Tripp, Jennifer A; McCullagh, James S O; Hedges, Robert E M

2006-01-01

Analysis of stable and radioactive isotopes from bone collagen provides useful information to archaeologists about the origin and age of bone artifacts. Isolation and analysis of single amino acids from the proteins can provide additional and more accurate information by removing contamination and separating a bulk isotope signal into its constituent parts. In this paper, we report a new method for the separation and isolation of underivatized amino acids from bone collagen, and their analysis by isotope ratio MS and accelerator MS. RP chromatography is used to separate the amino acids with nonpolar side chains, followed by an ion pair separation to isolate the remaining amino acids. The method produces single amino acids with little or no contamination from the separation process and allows for the measurement of accurate stable isotope ratios and pure samples for radiocarbon dating.

RECTIFIED ABSORPTION METHOD FOR THE SEPARATION OF HYDROGEN ISOTOPES

DOEpatents

Hunt, C.D.; Hanson, D.N.

1961-10-17

A method is described for separating and recovering heavy hydrogen isotopes from gaseous mixtures by multiple stage cyclic absorption and rectification from an approximate solvent. In particular, it is useful for recovering such isoteoes from ammonia feedstock streams containing nitrogen solvent. Modifications of the process ranging from isobaric to isothermal are provided. Certain impurities are tolerated, giving advantages over conventional fractional distillation processes. (AEC)

A status of progress for the Laser Isotope Separation (LIS) process

NASA Technical Reports Server (NTRS)

Delionback, L. M.

1976-01-01

An overview of the Laser Isotope Separation (LIS) methodology is given together with illustrations showing a simplified version of the LIS technique, an example of the two-photon photoionization category, and a diagram depicting how the energy levels of various isotope influence the LIS process. Applications were proposed for the LIS system which, in addition to enriching uranium, could in themselves develop into programs of tremendous scope and breadth. These include the treatment of radioactive wastes from light-water nuclear reactors, enriching the deuterium isotope to make heavy-water, and enriching the light isotopes of such elements as titanium for aerospace weight-reducing programs. Economic comparisons of the LIS methodology with the current method of gaseous diffusion indicate an overwhelming advantage; the laser process promises to be 1000 times more efficient. The technique could also be utilized in chemical reactions with the tuned laser serving as a universal catalyst to determine the speed and direction of a chemical reaction.

Advances in microscale separations towards nanoproteomics applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yi, Lian; Piehowski, Paul D.; Shi, Tujin

Microscale separations (e.g., liquid chromatography or capillary electrophoresis) coupled with mass spectrometry (MS) has become the primary tool for advanced proteomics, an indispensable technology for gaining understanding of complex biological processes. While significant advances have been achieved in MS-based proteomics, the current platforms still face a significant challenge in overall sensitivity towards nanoproteomics (i.e., with less than 1 g total amount of proteins available) applications such as cellular heterogeneity in tissue pathologies. Herein, we review recent advances in microscale separation techniques and integrated sample processing systems that improve the overall sensitivity and coverage of the proteomics workflow, and their contributionsmore » towards nanoproteomics applications.« less

Laser photochemical lead isotopes separation for harmless nuclear power engineering

NASA Astrophysics Data System (ADS)

Bokhan, P. A.; Fateev, N. V.; Kim, V. A.; Zakrevsky, D. E.

2016-09-01

The collisional quenching of the metastable 3 P 1,2 and 1 D 2 lead atoms is studied experimentally in the gas flow of the lead atoms, reagent-molecules and a carrier gas Ar. The experimental parameters were similar to the conditions that are required in the operation of the experimental setup for photochemical isotope separation. Excited atoms are generated under electron impact conditions created by a gas glow discharge through the mixture of gases and monitored photoelectrically by attenuation of atomic resonance radiation from hollow cathode 208Pb lamp. The decay of the excited atoms has been studied in the presence various molecules and total cross section data are reported. The flow tube measurements has allowed to separate the physical and chemical quenching channels and measure the rates of the chemical reaction excited lead with N2O, CH2Cl2, SF6 and CuBr molecules. These results are discussed in the prospects of the obtaining isotopically modified lead as a promising coolant in the reactors on the fast-neutron.

Mathematical modeling of filling of gas centrifuge cascade for nickel isotope separation by various feed flow rate

NASA Astrophysics Data System (ADS)

Ushakov, Anton; Orlov, Alexey; Sovach, Victor P.

2018-03-01

This article presents the results of research filling of gas centrifuge cascade for separation of the multicomponent isotope mixture with process gas by various feed flow rate. It has been used mathematical model of the nonstationary hydraulic and separation processes occurring in the gas centrifuge cascade. The research object is definition of the regularity transient of nickel isotopes into cascade during filling of the cascade. It is shown that isotope concentrations into cascade stages after its filling depend on variable parameters and are not equal to its concentration on initial isotope mixture (or feed flow of cascade). This assumption is used earlier any researchers for modeling such nonstationary process as set of steady-state concentration of isotopes into cascade. Article shows physical laws of isotope distribution into cascade stage after its filling. It's shown that varying each parameters of cascade (feed flow rate, feed stage number or cascade stage number) it is possible to change isotope concentration on output cascade flows (light or heavy fraction) for reduction of duration of further process to set of steady-state concentration of isotopes into cascade.

Aspects regarding at 13C isotope separation column control using Petri nets system

NASA Astrophysics Data System (ADS)

Boca, M. L.; Ciortea, M. E.

2015-11-01

This paper is intended to show that Petri nets can be also applicable in the chemical industry. It used linear programming, modeling underlying Petri nets, especially discrete event systems for isotopic separation, the purpose of considering and control events in real-time through graphical representations. In this paper it is simulate the control of 13C Isotope Separation column using Petri nets. The major problem with 13C comes from the difficulty of obtaining it and raising its natural fraction. Carbon isotopes can be obtained using many methods, one of them being the cryogenic distillation of carbon monoxide. Some few aspects regarding operating conditions and the construction of such cryogenic plants are known today, and even less information are available as far as the separation process modeling and control are concerned. In fact, the efficient control of the carbon monoxide distillation process represents a necessity for large-scale 13C production. Referring to a classic distillation process, some models for carbon isotope separation have been proposed, some based on mass, component and energy balance equations, some on the nonlinear wave theory or the Cohen equations. For modeling the system it was used Petri nets because in this case it is deal with discrete event systems. In use of the non-timed and with auxiliary times Petri model, the transport stream was divided into sections and these sections will be analyzed successively. Because of the complexity of the system and the large amount of calculations required it was not possible to analyze the system as a unitary whole. A first attempt to model the system as a unitary whole led to the blocking of the model during simulation, because of the large processing times.

Exploiting Diffusion Barrier and Chemical Affinity of Metal-Organic Frameworks for Efficient Hydrogen Isotope Separation.

PubMed

Kim, Jin Yeong; Balderas-Xicohténcatl, Rafael; Zhang, Linda; Kang, Sung Gu; Hirscher, Michael; Oh, Hyunchul; Moon, Hoi Ri

2017-10-25

Deuterium plays a pivotal role in industrial and scientific research, and is irreplaceable for various applications such as isotope tracing, neutron moderation, and neutron scattering. In addition, deuterium is a key energy source for fusion reactions. Thus, the isolation of deuterium from a physico-chemically almost identical isotopic mixture is a seminal challenge in modern separation technology. However, current commercial approaches suffer from extremely low separation efficiency (i.e., cryogenic distillation, selectivity of 1.5 at 24 K), requiring a cost-effective and large-scale separation technique. Herein, we report a highly effective hydrogen isotope separation system based on metal-organic frameworks (MOFs) having the highest reported separation factor as high as ∼26 at 77 K by maximizing synergistic effects of the chemical affinity quantum sieving (CAQS) and kinetic quantum sieving (KQS). For this purpose, the MOF-74 system having high hydrogen adsorption enthalpies due to strong open metal sites is chosen for CAQS functionality, and imidazole molecules (IM) are employed to the system for enhancing the KQS effect. To the best of our knowledge, this work is not only the first attempt to implement two quantum sieving effects, KQS and CAQS, in one system, but also provides experimental validation of the utility of this system for practical industrial usage by isolating high-purity D 2 through direct selective separation studies using 1:1 D 2 /H 2 mixtures.

Advances in primate stable isotope ecology-Achievements and future prospects.

PubMed

Crowley, Brooke E; Reitsema, Laurie J; Oelze, Vicky M; Sponheimer, Matt

2016-10-01

Stable isotope biogeochemistry has been used to investigate foraging ecology in non-human primates for nearly 30 years. Whereas early studies focused on diet, more recently, isotopic analysis has been used to address a diversity of ecological questions ranging from niche partitioning to nutritional status to variability in life history traits. With this increasing array of applications, stable isotope analysis stands to make major contributions to our understanding of primate behavior and biology. Most notably, isotopic data provide novel insights into primate feeding behaviors that may not otherwise be detectable. This special issue brings together some of the recent advances in this relatively new field. In this introduction to the special issue, we review the state of isotopic applications in primatology and its origins and describe some developing methodological issues, including techniques for analyzing different tissue types, statistical approaches, and isotopic baselines. We then discuss the future directions we envision for the field of primate isotope ecology. Am. J. Primatol. 78:995-1003, 2016. © 2015 Wiley Periodicals, Inc. © 2015 Wiley Periodicals, Inc.

Advances in microscale separations towards nanoproteomics applications

DOE PAGES

Yi, Lian; Piehowski, Paul D.; Shi, Tujin; ...

2017-07-21

Microscale separation (e.g., liquid chromatography or capillary electrophoresis) coupled with mass spectrometry (MS) has become the primary tool for advanced proteomics, an indispensable technology for gaining understanding of complex biological processes. In recent decades significant advances have been achieved in MS-based proteomics. But, the current proteomics platforms still face an analytical challenge in overall sensitivity towards nanoproteomics applications for starting materials of less than 1 μg total proteins (e.g., cellular heterogeneity in tissue pathologies). We review recent advances in microscale separation techniques and integrated sample processing strategies that improve the overall sensitivity and proteome coverage of the proteomics workflow, andmore » their contributions towards nanoproteomics applications.« less

Advances in microscale separations towards nanoproteomics applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yi, Lian; Piehowski, Paul D.; Shi, Tujin

Microscale separation (e.g., liquid chromatography or capillary electrophoresis) coupled with mass spectrometry (MS) has become the primary tool for advanced proteomics, an indispensable technology for gaining understanding of complex biological processes. In recent decades significant advances have been achieved in MS-based proteomics. But, the current proteomics platforms still face an analytical challenge in overall sensitivity towards nanoproteomics applications for starting materials of less than 1 μg total proteins (e.g., cellular heterogeneity in tissue pathologies). We review recent advances in microscale separation techniques and integrated sample processing strategies that improve the overall sensitivity and proteome coverage of the proteomics workflow, andmore » their contributions towards nanoproteomics applications.« less

Highly effective hydrogen isotope separation in nanoporous metal-organic frameworks with open metal sites: direct measurement and theoretical analysis.

PubMed

Oh, Hyunchul; Savchenko, Ievgeniia; Mavrandonakis, Andreas; Heine, Thomas; Hirscher, Michael

2014-01-28

Separating gaseous mixtures that consist of very similar size is one of the critical issues in modern separation technology. Especially, the separation of the isotopes hydrogen and deuterium requires special efforts, even though these isotopes show a very large mass ratio. Conventionally, H/D separation can be realized through cryogenic distillation of the molecular species or the Girdler-sulfide process, which are among the most energy-intensive separation techniques in the chemical industry. However, costs can be significantly reduced by using highly mass-selective nanoporous sorbents. Here, we describe a hydrogen isotope separation strategy exploiting the strongly attractive open metal sites present in nanoporous metal-organic frameworks of the CPO-27 family (also referred to as MOF-74). A theoretical analysis predicts an outstanding hydrogen isotopologue separation at open metal sites due to isotopal effects, which has been directly observed through cryogenic thermal desorption spectroscopy. For H2/D2 separation of an equimolar mixture at 60 K, the selectivity of 12 is the highest value ever measured, and this methodology shows extremely high separation efficiencies even above 77 K. Our theoretical results imply also a high selectivity for HD/H2 separation at similar temperatures, and together with catalytically active sites, we propose a mechanism to produce D2 from HD/H2 mixtures with natural or enriched deuterium content.

Advancing the Theory of Nuclear Reactions with Rare Isotopes: From the Laboratory to the Cosmos

DOE Office of Scientific and Technical Information (OSTI.GOV)

Elster, Charlotte

2015-06-01

The mission of the TORUS Topical Collaboration is to develop new methods that will advance nuclear reaction theory for unstable isotopes by using three-body techniques to improve direct-reaction calculations, and, by using a new partial-fusion theory, to integrate descriptions of direct and compound-nucleus reactions. Ohio University concentrates its efforts on the first part of the mission. Since direct measurements are often not feasible, indirect methods, e.g. (d,p) reactions, should be used. Those (d,p) reactions may be viewed as three-body reactions and described with Faddeev techniques. Faddeev equations in momentum space have a long tradition of utilizing separable interactions in ordermore » to arrive at sets of coupled integral equations in one variable. While there exist several separable representations for the nucleon-nucleon interaction, the optical potential between a neutron (proton) and a nucleus is not readily available in separable form. For this reason we first embarked in introducing a separable representation for complex phenomenological optical potentials of Woods-Saxon type.« less

MixSIAR: advanced stable isotope mixing models in R

EPA Science Inventory

Background/Question/Methods The development of stable isotope mixing models has coincided with modeling products (e.g. IsoSource, MixSIR, SIAR), where methodological advances are published in parity with software packages. However, while mixing model theory has recently been ex...

Modelling aspects regarding the control in 13C isotope separation column

NASA Astrophysics Data System (ADS)

Boca, M. L.

2016-08-01

Carbon represents the fourth most abundant chemical element in the world, having two stable and one radioactive isotope. The 13Carbon isotopes, with a natural abundance of 1.1%, plays an important role in numerous applications, such as the study of human metabolism changes, molecular structure studies, non-invasive respiratory tests, Alzheimer tests, air pollution and global warming effects on plants [9] A manufacturing control system manages the internal logistics in a production system and determines the routings of product instances, the assignment of workers and components, the starting of the processes on not-yet-finished product instances. Manufacturing control does not control the manufacturing processes themselves, but has to cope with the consequences of the processing results (e.g. the routing of products to a repair station). In this research it was fulfilled some UML (Unified Modelling Language) diagrams for modelling the C13 Isotope Separation column, implement in STARUML program. Being a critical process and needing a good control and supervising, the critical parameters in the column, temperature and pressure was control using some PLC (Programmable logic controller) and it was made some graphic analyze for this to observe some critical situation than can affect the separation process. The main parameters that need to be control are: -The liquid nitrogen (N2) level in the condenser. -The electrical power supplied to the boiler. -The vacuum pressure.

Photolytic separation of isotopes in cryogenic solution

DOEpatents

Freund, S.M.; Maier, W.B. II; Holland, R.F.; Battie, W.H.

Separation of carbon isotopes by photolysis of CS/sub 2/ in cryogenic solutions of nitrogen, krypton and argon with 206 nm light from an iodine resonance lamp is reported. The spectral distributionn of the ultraviolet absorption depends on solvent. Thus, in liquid nitrogen the photolytic decomposition rate of /sup 13/CS/sub 2/ is greater than that of /sup 12/CS/sub 2/ (because the absorption of 206 nm radiation is greater for /sup 13/CS/sub 2/), whereas in liquid krypton and liquid argon the reverse is true. The shift in ultraviolet spectrum is a general phenomenon readily characterized as a function of solvent polarizability, and exhibits behavior similar to that for vibrational transitions occurring in the infrared.

Photolytic separation of isotopes in cryogenic solution

DOEpatents

Freund, Samuel M.; Maier, II, William B.; Holland, Redus F.; Beattie, Willard H.

1985-01-01

Separation of carbon isotopes by photolysis of CS.sub.2 in cryogenic solutions of nitrogen, krypton and argon with 206 nm light from an iodine resonance lamp is reported. The spectral distribution of the ultraviolet absorption depends on solvent. Thus, in liquid nitrogen the photolytic decomposition rate of .sup.13 CS.sub.2 is greater than that of .sup.12 CS.sub.2 (because the absorption of 206 nm radiation is greater for .sup.13 CS.sub.2), whereas in liquid krypton and liquid argon the reverse is true. The shift in ultraviolet spectrum is a general phenomenon readily characterized as a function of solvent polarizability, and exhibits behavior similar to that for vibrational transitions occurring in the infrared.

Water isotope partitioning and ecohydrologic separation in mixed conifer forest explored with a centrifugation water extraction method

NASA Astrophysics Data System (ADS)

Bowers, W.; Mercer, J.; Pleasants, M.; Williams, D. G.

2017-12-01

Isotopic partitioning of water within soil into tightly and loosely bound fractions has been proposed to explain differences between isotopic water sources used by plants and those that contribute to streams and ground water, the basis for the "two water worlds" hypothesis. We examined the isotope ratio values of water in trees, bulk soil, mobile water collected from soil lysimeters, stream water, and GW at three different hillslopes in a mixed conifer forest in southeastern Wyoming, USA. Hillslopes differed in aspect and topographic position with corresponding differences in surface energy balance, snowmelt timing, and duration of soil moisture during the dry summer. The isotopic results support the partitioning of water within the soil; trees apparently used a different pool of water for transpiration than that recovered from soil lysimeters and the source was not resolved with the isotopic signature of the water that was extracted from bulk soil via cryogenic vacuum distillation. Separating and measuring the isotope ratios values in these pools would test the assumption that the tightly bound water within the soil has the same isotopic signature as the water transpired by the trees. We employed a centrifugation approach to separate water within the soil held at different tensions by applying stepwise increases in rotational velocity and pressures to the bulk soil samples. Effluent and the remaining water (cryogenically extracted) at each step were compared. We first applied the centrifugation method in a simple lab experiment using sandy loam soil and separate introductions of two isotopically distinct waters. We then applied the method to soil collected from the montane hillslopes. For the lab experiment, we predicted that effluents would have distinct isotopic signatures, with the last effluent and extracted water more closely representing the isotopic signature of the first water applied. For our field samples, we predicted that the isotopic signature of the

Isotopic separation of acetaldehyde and methanol from their deuterated isotopologues on a porous layer open tubular column allows quantification by stable isotope dilution without mass spectrometric detection.

PubMed

Schmarr, Hans-Georg; Wacker, Michael; Mathes, Maximilian

2017-01-20

An isotopic separation of acetaldehyde and acetaldehyde-2,2,2-d3 was achieved in a temperature programmed run on a porous layer open tubular (PLOT) capillary column coated with particles of divinylbenzene ethylene glycol/dimethylacrylate (Rt ® -U-BOND). This is the prerequisite for the development of quantitative analytical methods based on a stable isotope dilution assay (SIDA) without a mass spectrometric detection (non-MS SIDA). For routine analysis a flame ionization detector (FID) can thus be applied as a robust and low-cost alternative. In a preliminary study, static headspace extraction and gas chromatographic separation (HS-GC-FID) of acetaldehyde in aqueous solutions was shown as an application. Good linearity was obtained in a calibration range from 0.4 to 40mgL -1 , with peak integration benefitting from the inverse isotope effect encountered on the specific porous polymer. Furthermore, separation of methanol and deuterated methanol (d3) could also be achieved under the same chromatographic conditions. The achieved isotopic separation of these important volatile compounds now allows non-MS SIDA-based methods that are still to be developed. Copyright © 2016 Elsevier B.V. All rights reserved.

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/.

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.

Scalable and efficient separation of hydrogen isotopes using graphene-based electrochemical pumping

NASA Astrophysics Data System (ADS)

Lozada-Hidalgo, M.; Zhang, S.; Hu, S.; Esfandiar, A.; Grigorieva, I. V.; Geim, A. K.

2017-05-01

Thousands of tons of isotopic mixtures are processed annually for heavy-water production and tritium decontamination. The existing technologies remain extremely energy intensive and require large capital investments. New approaches are needed to reduce the industry's footprint. Recently, micrometre-size crystals of graphene are shown to act as efficient sieves for hydrogen isotopes pumped through graphene electrochemically. Here we report a fully-scalable approach, using graphene obtained by chemical vapour deposition, which allows a proton-deuteron separation factor of around 8, despite cracks and imperfections. The energy consumption is projected to be orders of magnitude smaller with respect to existing technologies. A membrane based on 30 m2 of graphene, a readily accessible amount, could provide a heavy-water output comparable to that of modern plants. Even higher efficiency is expected for tritium separation. With no fundamental obstacles for scaling up, the technology's simplicity, efficiency and green credentials call for consideration by the nuclear and related industries.

High-power CO laser with RF discharge for isotope separation employing condensation repression

NASA Astrophysics Data System (ADS)

Baranov, I. Ya.; Koptev, A. V.

2008-10-01

High-power CO laser can be the effective tool in such applications as isotope separation using the free-jet CRISLA method. The way of transfer from CO small-scale experimental installation to industrial high-power CO lasers is proposed through the use of a low-current radio-frequency (RF) electric discharge in a supersonic stream without an electron gun. The calculation model of scaling CO laser with RF discharge in supersonic stream was developed. The developed model allows to calculate parameters of laser installation and optimize them with the purpose of reception of high efficiency and low cost of installation as a whole. The technical decision of industrial CO laser for isotope separation employing condensation repression is considered. The estimated cost of laser is some hundred thousand dollars USA and small sizes of laser head give possibility to install it in any place.

Enhancement of Identity in the Hydraulic Characteristics of a Gas Centrifuge for Isotope Separation

NASA Astrophysics Data System (ADS)

Yatsenko, D. V.; Borisevich, V. D.; Godisov, O. N.

The problem of non-identity in characteristics of the GCs for uranium isotope separation grows up with increase of a rotor speed of rotation. It may lead to noticeable decrease of the separative power of the centrifugal machines. The carried out assessments allowed to get the dependence of the relative separation performance losses on the non-identity in the hydraulic characteristics of the GCs connected in parallel. The results of calculation are compared with that of obtained in experiments.

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.

Basic features of boron isotope separation by SILARC method in the two-step iterative static model

NASA Astrophysics Data System (ADS)

Lyakhov, K. A.; Lee, H. J.

2013-05-01

In this paper we develop a new static model for boron isotope separation by the laser assisted retardation of condensation method (SILARC) on the basis of model proposed by Jeff Eerkens. Our model is thought to be adequate to so-called two-step iterative scheme for isotope separation. This rather simple model helps to understand combined action on boron separation by SILARC method of all important parameters and relations between them. These parameters include carrier gas, molar fraction of BCl3 molecules in carrier gas, laser pulse intensity, gas pulse duration, gas pressure and temperature in reservoir and irradiation cells, optimal irradiation cell and skimmer chamber volumes, and optimal nozzle throughput. A method for finding optimal values of these parameters based on some objective function global minimum search was suggested. It turns out that minimum of this objective function is directly related to the minimum of total energy consumed, and total setup volume. Relations between nozzle throat area, IC volume, laser intensity, number of nozzles, number of vacuum pumps, and required isotope production rate were derived. Two types of industrial scale irradiation cells are compared. The first one has one large throughput slit nozzle, while the second one has numerous small nozzles arranged in parallel arrays for better overlap with laser beam. It is shown that the last one outperforms the former one significantly. It is argued that NO2 is the best carrier gas for boron isotope separation from the point of view of energy efficiency and Ar from the point of view of setup compactness.

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.

Laser separation of lithium isotopes by double resonance enhanced multiphoton ionization of Li/sub 2/

DOE Office of Scientific and Technical Information (OSTI.GOV)

Balz, J.G.; Bernheim, R.A.; Gold, L.P.

1987-01-01

Multiphoton ionization spectra of /sup 7/Li/sub 2/, /sup 6/Li/sub 2/, and /sup 7/Li/sup 6/Li vapors have been measured in the 570--650 nm region using a single, low resolution, multimode cw dye laser. A number of wavelengths provide selective multiphoton ionization of one isotopic species demonstrating the possibility of efficient laser-driven isotopic separation in lithium in this wavelength region.

Isotopic determinations of rhenium and osmium in meteorites by using fusion, distillation and ion-exchange separations

USGS Publications Warehouse

Morgan, J.W.; Walker, R.J.

1989-01-01

A stable isotope-dilution method using resonance ionization mass spectrometry is suitable for the determination of rhenium and osmium abundances and osmium isotopic composition in carbonaceous chondrites and iron meteorites. The chemical procedure involves sodium peroxide fusion, followed by distillation of osmium from sulfuric acid/hydrogen peroxide and subsequent anion-exchange separation of rhenium from the same solution. ?? 1989.

Hydrogen isotope systematics of phase separation in submarine hydrothermal systems: Experimental calibration and theoretical models

USGS Publications Warehouse

Berndt, M.E.; Seal, R.R.; Shanks, Wayne C.; Seyfried, W.E.

1996-01-01

Hydrogen isotope fractionation factors were measured for coexisting brines and vapors formed by phase separation of NaCl/H2O fluids at temperatures ranging from 399-450??C and pressures from 277-397 bars. It was found that brines are depleted in D compared to coexisting vapors at all conditions studied. The magnitude of hydrogen isotope fractionation is dependent on the relative amounts of Cl in the two phases and can be empirically correlated to pressure using the following relationship: 1000 ln ??(vap-brine) = 2.54(??0.83) + 2.87(??0.69) x log (??P), where ??(vap-brine) is the fractionation factor and ??P is a pressure term representing distance from the critical curve in the NaCl/H2O system. The effect of phase separation on hydrogen isotope distribution in subseafloor hydrothermal systems depends on a number of factors, including whether phase separation is induced by heating at depth or by decompression of hydrothermal fluids ascending to the seafloor. Phase separation in most subseafloor systems appears to be a simple process driven by heating of seawater to conditions within the two-phase region, followed by segregation and entrainment of brine or vapor into a seawater dominated system. Resulting vent fluids exhibit large ranges in Cl concentration with no measurable effect on ??D. Possible exceptions to this include hydrothermal fluids venting at Axial and 9??N on the East Pacific Rise. High ??D values of low Cl fluids venting at Axial are consistent with phase separation taking place at relatively shallow levels in the oceanic crust while negative ??D values in some low Cl fluids venting at 9??N suggest involvement of a magmatic fluid component or phase separation of D-depleted brines derived during previous hydrothermal activity.

New triple oxygen isotope data of bulk and separated fractions from SNC meteorites: Evidence for mantle homogeneity of Mars

NASA Astrophysics Data System (ADS)

Ali, Arshad; Jabeen, Iffat; Gregory, David; Verish, Robert; Banerjee, Neil R.

2016-05-01

We report precise triple oxygen isotope data of bulk materials and separated fractions of several Shergotty-Nakhla-Chassigny (SNC) meteorites using enhanced laser-assisted fluorination technique. This study shows that SNCs have remarkably identical Δ17O and a narrow range in δ18O values suggesting that these meteorites have assimilated negligibly small surface materials (<5%), which is undetectable in the oxygen isotope compositions reported here. Also, fractionation factors in coexisting silicate mineral pairs (px-ol and mask-ol) further demonstrate isotopic equilibrium at magmatic temperatures. We present a mass-dependent fractionation line for bulk materials with a slope of 0.526 ± 0.016 (1SE) comparable to the slope obtained in an earlier study (0.526 ± 0.013; Franchi et al. 1999). We also present a new Martian fractionation line for SNCs constructed from separated fractions (i.e., pyroxene, olivine, and maskelynite) with a slope of 0.532 ± 0.009 (1SE). The identical fractionation lines run above and parallel to our terrestrial fractionation line with Δ17O = 0.318 ± 0.016‰ (SD) for bulk materials and 0.316 ± 0.009‰ (SD) for separated fractions. The conformity in slopes and Δ17O between bulk materials and separated fractions confirm oxygen isotope homogeneity in the Martian mantle though recent studies suggest that the Martian lithosphere may potentially have multiple oxygen isotope reservoirs.

Preliminary results from a microvolume, dynamically heated analytical column for preconcentration and separation of simple gases prior to stable isotopic analysis

NASA Astrophysics Data System (ADS)

Panetta, Robert James; Seed, Mike

2016-04-01

Stable isotope applications that call for preconcentration (i.e., greenhouse gas measurements, small carbonate samples, etc.) universally call for cryogenic fluids such as liquid nitrogen, dry ice slurries, or expensive external recirculation chillers. This adds significant complexity, first and foremost in the requirements to store and handle such dangerous materials. A second layer of complexity is the instrument itself - with mechanisms to physically move either coolant around the trap, or move a trap in or out of the coolant. Not to mention design requirements for hardware that can safely isolate the fluid from other sensitive areas. In an effort to simplify the isotopic analysis of gases requiring preconcentration, we have developed a new separation technology, UltiTrapTM (patent pending), which leverage's the proprietary Advanced Purge & Trap (APT) Technology employed in elemental analysers from Elementar Analysensysteme GmbH products. UltiTrapTM has been specially developed as a micro volume, dynamically heated GC separation column. The introduction of solid-state cooling technology enables sub-zero temperatures without cryogenics or refrigerants, eliminates all moving parts, and increases analytical longevity due to no boiling losses of coolant . This new technology makes it possible for the system to be deployed as both a focussing device and as a gas separation device. Initial data on synthetic gas mixtures (CO2/CH4/N2O in air), and real-world applications including long-term room air and a comparison between carbonated waters of different origins show excellent agreement with previous technologies.

Separated isotopes: Vital tools for science and medicine

NASA Astrophysics Data System (ADS)

Deliberations and conclusions of a workshop on stable isotopes and derived radioisotopes organized by the Subcommittee on Nuclear and Radiochemistry of the National Research Council's Committee on Chemical Sciences at the request of the Department of Energy (DOE) are summarized. The workshop was jointly supported by the National Institutes of Health and DOE's Office of Basic Energy Sciences. An overview with three recommendations resulting from the workshop is followed by reports of the four workshop panels. Background papers were prepared by individuals on the Steering Committee and made available to all participants prior to the Workshop. They are reproduced as Appendixes 3 to 8. Short reports on alternate separation techniques were presented at the Workshop and are reproduced in Appendixes 9 to 11.

Cryogenic separation of an oxygen-argon mixture in natural air samples for the determination of isotope and molecular ratios.

PubMed

Keedakkadan, Habeeb Rahman; Abe, Osamu

2015-04-30

The separation and purification of oxygen-argon mixtures are critical in the high-precision analysis of Δ(17) O and δ(O2 /Ar) for geochemical applications. At present, chromatographic methods are used for the separation and purification of oxygen-argon mixtures or pure oxygen, but these methods require the use of high-purity helium as a carrier gas. Considerable interest has been expressed in the development of a helium-free cryogenic separation of oxygen-argon mixtures in natural air samples. The precise and simplified cryogenic separation of oxygen-argon mixtures from natural air samples presented here was made possible using a single 5A (30/60 mesh) molecular sieve column. The method involves the trapping of eluted gases using molecular sieves at liquid nitrogen temperature, which is associated with isotopic fractionation. We tested the proposed method for the determination of isotopic fractionations during the gas exchange between water and atmospheric air at equilibrium. The dependency of fractionation was studied at different water temperatures and for different methods of equilibration (bubbling and stirring). Isotopic and molecular fractionations during gas desorption from molecular sieves were studied for different amounts and types of molecular sieves. Repeated measurements of atmospheric air yielded a reproducibility (±SD) of 0.021 ‰, 0.044 ‰, 15 per meg and 1.9 ‰ for δ(17) O, δ(18) O, Δ(17) O and δ(O2 /Ar) values, respectively. We applied the method to determine equilibrium isotope fractionation during gas exchange between air and water. Consistent δ(18) O and Δ(17) O results were obtained with the latest two studies, whereas there was a significant difference in δ(18) O values between seawater and deionized water. We have revised a helium-free, cryogenic separation of oxygen-argon mixtures in natural air samples for isotopic and molecular ratio analysis. The use of a single 13X (1/8" pellet) molecular sieve yielded the smallest isotopic

Advances in the measurement of sulfur isotopes by multi-collector ICP-MS (MC-ICP- MS)

NASA Astrophysics Data System (ADS)

Ridley, W. I.; Wilson, S. A.; Anthony, M. W.

2006-12-01

The demonstrated capability to measure 34S/32S by MC-ICP-MS with a precision (2ó) of ~0.2 per mil has many potential applications in geochemistry. However, a number of obstacles limit this potential. First, to achieve the precision indicated above requires sufficient mass resolution to separate isobaric interferences of 16O2 and 17O2 on 32S and 34S, respectively. These requirements for high resolution mean overall instrument sensitivity is reduced. Second, current methods preclude analysis of samples with complex matrices, a common characteristic of sulfur-bearing geologic materials. Here, we describe and discuss a method that provides both efficient removal of matrix constituents, and provides pre-concentration of S, thus overcoming these obstacles. The method involves the separation of sulfur from matrix constituents by high pressure (1000 psi) ion chromatography (HPIC), followed by isotope measurement using MC-ICP-MS. This combination allows for analysis of liquid samples with a wide range of S concentrations. A powerful advantage of this technique is the efficient separation of many sulfur species from matrix cations and anions (for instance in a seawater or acid mine drainage matrix), as well as the separation of sulfur species, e.g., sulfate, sulfite, thiosulfate, thiocynate, from each other for isotope analysis. The automated HPIC system uses a carbonate-bicarbonate eluent with eluent suppression, and has sufficient baseline separation to collect the various sulfur species as pure fractions. The individual fractions are collected over a specific time interval based upon a pre-determined elution profile and peak retention times. The addition of a second ion exchange column into the system allows pre-concentration of sulfur species by 2-3 orders of magnitude for samples that otherwise would have sulfur concentrations too low to provide precise isotopic ratios. The S isotope ratios are measured by MC-ICP-MS using a desolvating sample introduction system, a

Chromatographic Separation of Cd from Plants via Anion-Exchange Resin for an Isotope Determination by Multiple Collector ICP-MS.

PubMed

Wei, Rongfei; Guo, Qingjun; Wen, Hanjie; Peters, Marc; Yang, Junxing; Tian, Liyan; Han, Xiaokun

2017-01-01

In this study, key factors affecting the chromatographic separation of Cd from plants, such as the resin column, digestion and purification procedures, were experimentally investigated. A technique for separating Cd from plant samples based on single ion-exchange chromatography has been developed, which is suitable for the high-precision analysis of Cd isotopes by multiple-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). The robustness of the technique was assessed by replicate analyses of Cd standard solutions and plant samples. The Cd yields of the whole separation process were higher than 95%, and the 114/110 Cd values of three Cd second standard solutions (Münster Cd, Spex Cd, Spex-1 Cd solutions) relative to the NIST SRM 3108 were measured accurately, which enabled the comparisons of Cd isotope results obtained in other laboratories. Hence, stable Cd isotope analyses represent a powerful tool for fingerprinting specific Cd sources and/or examining biogeochemical reactions in ecological and environmental systems.

Separated isotopes: vital tools for science and medicine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1982-01-01

Deliberations and conclusions of a Workshop on Stable Isotopes and Derived Radioisotopes organized by the Subcommittee on Nuclear and Radiochemistry of the National Research Council's Committee on Chemical Sciences at the request of the Department of Energy (DOE) are summarized. The workshop was jointly supported by the National Institutes of Health and DOE's Office of Basic Energy Sciences. An overview with three recommendations resulting from the Workshop is followed by reports of the four Workshop panels. Background papers were prepared by individuals on the Steering Committee and made available to all participants prior to the Workshop. They are reproduced asmore » Appendixes 3 to 8. Short reports on alternate separation techniques were presented at the Workshop and are reproduced in Appendixes 9 to 11.« less

Advanced flight hardware for organic separations

NASA Astrophysics Data System (ADS)

Deuser, Mark S.; Vellinger, John C.; Weber, John T.

1997-01-01

Aqueous Two-Phase Partitioning (ATPP) is a unique separation technique which allows purification and classification of biological materials. SHOT has employed the ATPP process in separation equipment developed for both space and ground applications. Initial equipment development and research focused on the ORganic SEParation (ORSEP) space flight experiments that were performed on suborbital rockets and the shuttle. ADvanced SEParations (ADSEP) technology was developed as the next generation of ORSEP equipment through a NASA Small Business Innovation Research (SBIR) contract. Under the SBIR contract, a marketing study was conducted, indicating a growing commercial market exists among biotechnology firms for ADSEP equipment and associated flight research and development services. SHOT is preparing to begin manufacturing and marketing laboratory versions of the ADSEP hardware for the ground-based market. In addition, through a self-financed SBIR Phase III effort, SHOT fabricated and integrated the ADSEP flight hardware for a commercially-driven flight experiment as the initial step in marketing space processing services. The ADSEP ground-based and microgravity research is expected to play a vital role in developing important new biomedical and pharmaceutical products.

Separation of the Isotopes of Calcium by Countercurrent Electromigration in Fused Salts. Final Report; SEPARATION DES ISOTOPES DU CALCIUM PAR ELECTROMIGRATION A CONTRE COURANT EN SELS FONDUS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Menes, F.; Dirian, G.

1962-12-14

The results obtained up to June 25, 1962, on the separation of Ca isotopes by electromigration in fused salts have been reported in seven progress reports. The data given in these reports are summarized. Later study investigated the improvement of the diaphragm performance using nonclassical methods, preparation of an experiment confirming the performances of the high capacity U tube'' apparatus, and preparation of an installation designed for perfecting the dropping tube'' device. Only preliminary results on these studes are available. (J.S.R.)

New design studies for TRIUMF's ARIEL High Resolution Separator

NASA Astrophysics Data System (ADS)

Maloney, J. A.; Baartman, R.; Marchetto, M.

2016-06-01

As part of its new Advanced Rare IsotopE Laboratory (ARIEL), TRIUMF is designing a novel High Resolution Separator (HRS) (Maloney et al., 2015) to separate rare isotopes. The HRS has a 180° bend, separated into two 90° magnetic dipoles, bend radius 1.2 m, with an electrostatic multipole corrector between them. Second order correction comes mainly from the dipole edge curvatures, but is intended to be fine-tuned with a sextupole component and a small octupole component in the multipole. This combination is designed to achieve 1:20,000 resolution for a 3 μm (horizontal) and 6 μm (vertical) emittance. A design for the HRS dipole magnets achieves both radial and integral flatness goals of <10-5. A review of the optical design for the HRS is presented, including the study of limiting factors affecting separation, matching and aberration correction. Field simulations from the OPERA-3D (OPERA) [2] models of the dipole magnets are used in COSY Infinity (COSY) (Berz and Makino, 2005) [3] to find and optimize the transfer maps to 3rd order and study residual nonlinearities to 8th order.

Simulation and Analysis of Isotope Separation System for Fusion Fuel Recovery System

NASA Astrophysics Data System (ADS)

Senevirathna, Bathiya; Gentile, Charles

2011-10-01

This paper presents results of a simulation of the Fuel Recovery System (FRS) for the Laser Inertial Fusion Engine (LIFE) reactor. The LIFE reaction will produce exhaust gases that will need to be recycled in the FRS along with xenon, the chamber's intervention gas. Solids and liquids will first be removed and then vapor traps are used to remove large gas molecules such as lead. The gas will be reacted with lithium at high temperatures to extract the hydrogen isotopes, protium, deuterium, and tritium in hydride form. The hydrogen isotopes will be recovered using a lithium blanket processing system already in place and this product will be sent to the Isotope Separation System (ISS). The ISS will be modeled in software to analyze its effectiveness. Aspen HYSYS was chosen for this purpose for its widespread use industrial gas processing systems. Reactants and corresponding chemical reactions had to be initialized in the software. The ISS primarily consists of four cryogenic distillation columns and these were modeled in HYSYS based on design requirements. Fractional compositions of the distillate and liquid products were analyzed and used to optimize the overall system.

Oxygen Isotopes Archived in Subfossil Chironomids: Advancing a Promising Proxy for Lake Water Isotopes

NASA Astrophysics Data System (ADS)

Lasher, G. E.; Axford, Y.; Blair, N. E.

2017-12-01

Oxygen isotopes measured in subfossil chironomid head capsules (aquatic insect remains) in lake sediments are beginning to offer paleoclimate insights from previously under-studied areas of the world. Since the first published pilot study demonstrated the potential of chironomid δ18O to record lake water δ18O (Wooller et al., 2004), subsequent work has refined our understanding of this proxy: confirming via lab cultures that growth water controls head capsule δ18O (Wang et al., 2009), refining laboratory pretreatment protocols, and further validating the method by demonstrating strong agreement between carbonate and chironomid-derived paleo-isotope records (Verbruggen et al., 2009, 2010, 2011). However, outstanding questions remain, including the seasonality of chironomid growth, possible species-dependent vital effects, and diagenetic effects on the protein-chitin complex that comprise chironomid cuticles. To address some of these questions, we summarize available data from paired modern chironomid-lake water δ18O values from around the world and discuss climatic and environmental factors affecting chironomid isotopic signatures. We also present new data on the resistance of these subfossils to diagenesis and degradation throughout the late Quaternary using Fourier Transform Infrared Spectroscopy (FT-IR) and Pyrolysis Gas Chromatography Mass Spectrometry (Py-GC/MS) of chironomid remains up to >100,000 years old. As chironomids are nearly ubiquitous in lakes globally and, we argue, molecularly stable through glacial and interglacial cycles, this proxy has the potential to greatly expand the spatial and temporal resolution of Quaternary paleo-isotopes and thus climate records. In addition to reviewing and presenting new methodological advances, we also present applications of chironomid δ18O from millennial- to centennial-scale Holocene Greenland lake records.

A modified lead-matrix separation procedure shown for lead isotope analysis in Trojan silver artefacts as an example.

PubMed

Vogl, Jochen; Paz, Boaz; Koenig, Maren; Pritzkow, Wolfgang

2013-03-01

A modified Pb-matrix separation procedure using NH4HCO3 solution as eluent has been developed and validated for determination of Pb isotope amount ratios by thermal ionization mass spectrometry. The procedure is based on chromatographic separation using the Pb·Spec resin and an in-house-prepared NH4HCO3 solution serving as eluent. The advantages of this eluent are low Pb blanks (<40 pg mL(-1)) and the property that NH4HCO3 can be easily removed by use of a heating step (>60 °C). Pb recovery is >95 % for water samples. For archaeological silver samples, however, the Pb recovery is reduced to approximately 50 %, but causes no bias in the determination of Pb isotope amount ratios. The validated procedure was used to determine lead isotope amount ratios in Trojan silver artefacts with expanded uncertainties (k = 2) <0.09 %.

Advanced Elemental and Isotopic Characterization of Atmospheric Aerosols

NASA Astrophysics Data System (ADS)

Shafer, M. M.; Schauer, J. J.; Park, J.

2001-12-01

Recent sampling and analytical developments advanced by the project team enable the detailed elemental and isotopic fingerprinting of extremely small masses of atmospheric aerosols. Historically, this type of characterization was rarely achieved due to limitations in analytical sensitivity and a lack of awareness concerning the potential for contamination. However, with the introduction of 3rd and 4th generation ICP-MS instrumentation and the application of state-of-the- art "clean-techniques", quantitative analysis of over 40 elements in sub-milligram samples can be realized. When coupled with an efficient and validated solubilization method, ICP-MS approaches provide distinct advantages in comparison with traditional methods; greatly enhanced detection limits, improved accuracy, and isotope resolution capability, to name a few. Importantly, the ICP-MS approach can readily be integrated with techniques which enable phase differentiation and chemical speciation information to be acquired. For example, selective chemical leaching can provide data on the association of metals with major phase-components, and oxidation state of certain metals. Critical information on metal-ligand stability can be obtained when electrochemical techniques, such as adsorptive cathodic stripping voltammetry (ACSV), are applied to these same extracts. Our research group is applying these techniques in a broad range of research projects to better understand the sources and distribution of trace metals in particulate matter in the atmosphere. Using examples from our research, including recent Pb and Sr isotope ratio work on Asian aerosols, we will illustrate the capabilities and applications of these new methods.

Selective Hydrogen Isotope Separation via Breathing Transition in MIL-53(Al).

PubMed

Kim, Jin Yeong; Zhang, Linda; Balderas-Xicohténcatl, Rafael; Park, Jaewoo; Hirscher, Michael; Moon, Hoi Ri; Oh, Hyunchul

2017-12-13

Breathing of MIL-53(Al), a flexible metal-organic framework (MOF), leads to dynamic changes as narrow pore (np) transitions to large pore (lp). During the flexible and reversible transition, the pore apertures are continuously adjusted, thus providing the tremendous opportunity to separate mixtures of similar-sized and similar-shaped molecules that require precise pore tuning. Herein, for the first time, we report a strategy for effectively separating hydrogen isotopes through the dynamic pore change during the breathing of MIL-53(Al), a representative of flexible MOFs. The experiment shows that the selectivity for D 2 over H 2 is strongly related to the state of the pore structure of MIL-53(Al). The highest selectivity (S D 2 /H 2 = 13.6 at 40 K) was obtained by optimizing the exposure temperature, pressure, and time to systematically tune the pore state of MIL-53(Al).

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.

Determination of Plutonium Isotope Ratios at Very Low Levels by ICP-MS using On-Line Electrochemically Modulated Separations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liezers, Martin; Lehn, Scott A; Olsen, Khris B

2009-10-01

Electrochemically modulated separations (EMS) are shown to be a rapid and selective means of extracting and concentrating Pu from complex solutions prior to isotopic analysis by inductively coupled plasma mass spectrometry (ICP-MS). This separation is performed in a flow injection mode, on-line with the ICP-MS. A three-electrode, flow-by electrochemical cell is used to accumulate Pu at an anodized glassy carbon electrode by redox conversion of Pu(III) to Pu (IV&VI). The entire process takes place in 2% v/v (0.46M) HNO 3. No redox chemicals or acid concentration changes are required. Plutonium accumulation and release is redox dependent and controlled by themore » applied cell potential. Thus large transient volumetric concentration enhancements can be achieved. Based on more negative U(IV) potentials relative to Pu(IV), separation of Pu from uranium is efficient, thereby eliminating uranium hydride interferences. EMS-ICP-MS isotope ratio measurement performance will be presented for femtogram to attogram level plutonium concentrations.« less

Numerical modelling of the flow and isotope separation in centrifuge Iguasu for different lengths of the rotor

NASA Astrophysics Data System (ADS)

Bogovalov, S. V.; Borisevich, V. D.; Borman, V. D.; Tronin, I. V.; Tronin, V. N.

2016-06-01

Numerical modelling and optimization of the gas flow and isotope separation in the Iguasu gas centrifuge (GC) for uranium enrichment have been performed for different lengths of the rotor. The calculations show that the specific separative power of the GC reduces with the length of the rotor. We show that the reduction of the specific separative power is connected with the growth of the pressure in the optimal regime and corresponding growth of temperature to prevent the working gas sublimation. The specific separative power remains constant with the growth of the rotor length provided that the temperature of the gas is taken to be constant.

Numerical modelling of the flow and isotope separation in centrifuge Iguasu for different lengths of the rotor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bogovalov, S. V.; Borisevich, V. D.; Borman, V. D.

Numerical modelling and optimization of the gas flow and isotope separation in the Iguasu gas centrifuge (GC) for uranium enrichment have been performed for different lengths of the rotor. The calculations show that the specific separative power of the GC reduces with the length of the rotor. We show that the reduction of the specific separative power is connected with the growth of the pressure in the optimal regime and corresponding growth of temperature to prevent the working gas sublimation. The specific separative power remains constant with the growth of the rotor length provided that the temperature of the gasmore » is taken to be constant.« less

Battery Separator Characterization and Evaluation Procedures for NASA's Advanced Lithium-Ion Batteries

NASA Technical Reports Server (NTRS)

Baldwin, Richard S.; Bennet, William R.; Wong, Eunice K.; Lewton, MaryBeth R.; Harris, Megan K.

2010-01-01

To address the future performance and safety requirements for the electrical energy storage technologies that will enhance and enable future NASA manned aerospace missions, advanced rechargeable, lithium-ion battery technology development is being pursued within the scope of the NASA Exploration Technology Development Program s (ETDP's) Energy Storage Project. A critical cell-level component of a lithium-ion battery which significantly impacts both overall electrochemical performance and safety is the porous separator that is sandwiched between the two active cell electrodes. To support the selection of the optimal cell separator material(s) for the advanced battery technology and chemistries under development, laboratory characterization and screening procedures were established to assess and compare separator material-level attributes and associated separator performance characteristics.

High‐precision determination of lithium and magnesium isotopes utilising single column separation and multi‐collector inductively coupled plasma mass spectrometry

PubMed Central

Misra, Sambuddha; Lloyd, Nicholas; Elderfield, Henry; Bickle, Mike J.

2017-01-01

Rationale Li and Mg isotopes are increasingly used as a combined tool within the geosciences. However, established methods require separate sample purification protocols utilising several column separation procedures. This study presents a single‐step cation‐exchange method for quantitative separation of trace levels of Li and Mg from multiple sample matrices. Methods The column method utilises the macro‐porous AGMP‐50 resin and a high‐aspect ratio column, allowing quantitative separation of Li and Mg from natural waters, sediments, rocks and carbonate matrices following the same elution protocol. High‐precision isotope determination was conducted by multi‐collector inductively coupled plasma mass spectrometry (MC‐ICPMS) on the Thermo Scientific™ NEPTUNE Plus™ fitted with 1013 Ω amplifiers which allow accurate and precise measurements at ion beams ≤0.51 V. Results Sub‐nanogram Li samples (0.3–0.5 ng) were regularly separated (yielding Mg masses of 1–70 μg) using the presented column method. The total sample consumption during isotopic analysis is <0.5 ng Li and <115 ng Mg with long‐term external 2σ precisions of ±0.39‰ for δ7Li and ±0.07‰ for δ26Mg. The results for geological reference standards and seawater analysed by our method are in excellent agreement with published values despite the order of magnitude lower sample consumption. Conclusions The possibility of eluting small sample masses and the low analytical sample consumption make this method ideal for samples of limited mass or low Li concentration, such as foraminifera, mineral separates or dilute river waters. PMID:29078008

Ion exchange separation of chromium from natural water matrix for stable isotope mass spectrometric analysis

USGS Publications Warehouse

Ball, J.W.; Bassett, R.L.

2000-01-01

A method has been developed for separating the Cr dissolved in natural water from matrix elements and determination of its stable isotope ratios using solid-source thermal-ionization mass spectrometry (TIMS). The separation method takes advantage of the existence of the oxidized form of Cr as an oxyanion to separate it from interfering cations using anion-exchange chromatography, and of the reduced form of Cr as a positively charged ion to separate it from interfering anions such as sulfate. Subsequent processing of the separated sample eliminates residual organic material for application to a solid source filament. Ratios for 53Cr/52Cr for National Institute of Standards and Technology Standard Reference Material 979 can be measured using the silica gel-boric acid technique with a filament-to-filament standard deviation in the mean 53Cr/52Cr ratio for 50 replicates of 0.00005 or less. (C) 2000 Elsevier Science B.V. All rights reserved.

Evaluation of carbon isotope flux partitioning theory under simplified and controlled environmental conditions

USDA-ARS?s Scientific Manuscript database

Separation of the photosynthetic (Fp) and respiratory (Fr) fluxes of net CO2 exchange (Fn)remains a necessary step toward understanding the biological and physical controls on carbon cycling between the soil, biomass, and atmosphere. Despite recent advancements in stable carbon isotope partitioning ...

Separated isotopes: vital tools for science and medicine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1982-01-01

This report summarizes the deliberations and conclusions of a Workshop on Stable Isotopes and Derived Radioisotopes organized by the Subcommittee on Nuclear and Radiochemistry of the National Research Council's Committee on Chemical Sciences at the request of the Department of Energy (DOE). The workshop was jointly supported by the National Institutes of Health and DOE's Office of Basic Energy Sciences. An Overview with three recommendations resulting from the Workshop, prepared by the Steering Committee, is followed by Chapters 1 to 4, reports of the following four Workshop panels: (1) panel on research applications in physics, chemistry and geoscience; (2) panelmore » on commercial applications; (3) panel on biomedical research applications; (4) panel on clinical applications. Background papers were prepared by individuals on the Steering Committee and made available to all participants prior to the Workshop. They proved of great value and are reproduced as Appendixes 3 to 8. Short reports on alternate separation techniques were presented at the Workshop and are reproduced in Appendixes 9 to 11. Selected papers have been abstracted and indexed.« less

Isotope separation by selective charge conversion and field deflection

DOEpatents

Hickman, Robert G.

1978-01-01

A deuterium-tritium separation system wherein a source beam comprised of positively ionized deuterium (D.sup.+) and tritium (T.sup.+) is converted at different charge-exchange cell sections of the system to negatively ionized deuterium (D.sup.-) and tritium (T.sup.-). First, energy is added to the beam to accelerate the D.sup.+ ions to the velocity that is optimum for conversion of the D.sup.+ ions to D.sup.- ions in a charge-exchange cell. The T.sup.+ ions are accelerated at the same time, but not to the optimum velocity since they are heavier than the D.sup.+ ions. The T.sup.+ ions are, therefore, not converted to T.sup.- ions when the D.sup.+ ions are converted to D.sup.- ions. This enables effective separation of the beam by deflection of the isotopes with an electrostatic field, the D.sup.- ions being deflected in one direction and the T.sup.+ ions being deflected in the opposite direction. Next, more energy is added to the deflected beam of T.sup.+ ions to bring the T.sup.+ ions to the optimum velocity for their conversion to T.sup.- ions. In a particular use of the invention, the beams of D.sup.- and T.sup.- ions are separately further accelerated and then converted to energetic neutral particles for injection as fuel into a thermonuclear reactor. The reactor exhaust of D.sup.+ and T.sup.+ and the D.sup.+ and T.sup.+ that was not converted in the respective sections is combined with the source beam and recycled through the system to increase the efficiency of the system.

Fast isotopic separation of 10 B and 11 B boric acid by capillary zone electrophoresis.

PubMed

Kamencev, Mikhail; Yakimova, Nina; Moskvin, Leonid; Kuchumova, Irina; Tkach, Kirill; Malinina, Yulia

2016-11-01

Fast isotopic separation of 10 B and 11 B boric acid by CZE was demonstrated. The BGE contained 25 mM phenylalanine and 5 mM putrescine (рН 8.95). The running conditions were +25 kV at 20°C with indirect photometric detection at 210 nm. Baseline separation was achieved in less than 9 min. RSD of migration times and corrected peak areas were less than 0.5 and 3%, respectively (n = 5). Linearity was demonstrated in the range 0.2-2 mM for 11 B and 0.2-0.5 mM for 10 B. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Establishment of the Center for Advanced Separation Technologies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Christopher E. Hull

2006-09-30

This Final Technical Report covers the eight sub-projects awarded in the first year and the five projects awarded in the second year of Cooperative Agreement DE-FC26-01NT41091: Establishment of the Center for Advanced Separation Technologies. This work is summarized in the body of the main report: the individual sub-project Technical Progress Reports are attached as Appendices.

Methods for the separation of rhenium, osmium and molybdenum applicable to isotope geochemistry

USGS Publications Warehouse

Morgan, J.W.; Golightly, D.W.; Dorrzapf, A.F.

1991-01-01

Effective methods are described for the chemical separation of rhenium, osmium and molybdenum. The methods are based on distillation and anion-exchange chromatography, and have been the basis for rhenium-osmium isotope studies of ore deposits and meteorites. Successful anion-exchange separation of osmium requires both recognition and careful control of the osmium species in solution; thus, distillation of osmium tetroxide from a mixture of sulfuric acid and hydrogen peroxide is preferred to anion-exchange. Distribution coefficients measured for perrhenate in sulfuric acid media are sufficiently high (Kd > 500) for rhenium to be directly loaded onto an ion-exchange column from a distillation residue and subsequently eluted with nitric acid. Polymerization of molybdenum species during elution is prevented by use of a solution that is 1M in hydrochloric acid and 1M in sodium chloride. ?? 1991.

Selective IR multiphoton dissociation of molecules in a pulsed gas-dynamically cooled molecular flow interacting with a solid surface as an alternative to low-energy methods of molecular laser isotope separation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Makarov, G N; Petin, A N

2016-03-31

We report the results of studies on the isotope-selective infrared multiphoton dissociation (IR MFD) of SF{sub 6} and CF{sub 3}I molecules in a pulsed, gas-dynamically cooled molecular flow interacting with a solid surface. The productivity of this method in the conditions of a specific experiment (by the example of SF{sub 6} molecules) is evaluated. A number of low-energy methods of molecular laser isotope separation based on the use of infrared lasers for selective excitation of molecules are analysed and their productivity is estimated. The methods are compared with those of selective dissociation of molecules in the flow interacting with amore » surface. The advantages of this method compared to the low-energy methods of molecular laser isotope separation and the IR MPD method in the unperturbed jets and flows are shown. It is concluded that this method could be a promising alternative to the low-energy methods of molecular laser isotope separation. (laser separation of isotopes)« less

Advancing the scientific basis of trivalent actinide-lanthanide separations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nash, K.L.

For advanced fuel cycles designed to support transmutation of transplutonium actinides, several options have been demonstrated for process-scale aqueous separations for U, Np, Pu management and for partitioning of trivalent actinides and fission product lanthanides away from other fission products. The more difficult mutual separation of Am/Cm from La-Tb remains the subject of considerable fundamental and applied research. The chemical separations literature teaches that the most productive alternatives to pursue are those based on ligand donor atoms less electronegative than O, specifically N- and S-containing complexants and chloride ion (Cl{sup -}). These 'soft-donor' atoms have exhibited usable selectivity in theirmore » bonding interactions with trivalent actinides relative to lanthanides. In this report, selected features of soft donor reagent design, characterization and application development will be discussed. The roles of thiocyanate, aminopoly-carboxylic acids and lactate in separation processes are detailed. (authors)« less

[Research advances in identifying nitrate pollution sources of water environment by using nitrogen and oxygen stable isotopes].

PubMed

Mao, Wei; Liang, Zhi-wei; Li, Wei; Zhu, Yao; Yanng, Mu-yi; Jia, Chao-jie

2013-04-01

Water body' s nitrate pollution has become a common and severe environmental problem. In order to ensure human health and water environment benign evolution, it is of great importance to effectively identify the nitrate pollution sources of water body. Because of the discrepant composition of nitrogen and oxygen stable isotopes in different sources of nitrate in water body, nitrogen and oxygen stable isotopes can be used to identify the nitrate pollution sources of water environment. This paper introduced the fractionation factors of nitrogen and oxygen stable isotopes in the main processes of nitrogen cycling and the composition of these stable isotopes in main nitrate sources, compared the advantages and disadvantages of five pre-treatment methods for analyzing the nitrogen and oxygen isotopes in nitrate, and summarized the research advances in this aspect into three stages, i. e. , using nitrogen stable isotope alone, using nitrogen and oxygen stable isotopes simultaneously, and combining with mathematical models. The future research directions regarding the nitrate pollution sources identification of water environment were also discussed.

Testing isotopic labeling with [¹³C₆]glucose as a method of advanced glycation sites identification.

PubMed

Kielmas, Martyna; Kijewska, Monika; Stefanowicz, Piotr; Szewczuk, Zbigniew

2012-12-01

The Maillard reaction occurring between reducing sugars and reactive amino groups of biomolecules leads to the formation of a heterogeneous mixture of compounds: early, intermediate, and advanced glycation end products (AGEs). These compounds could be markers of certain diseases and of the premature aging process. Detection of Amadori products can be performed by various methods, including MS/MS techniques and affinity chromatography on immobilized boronic acid. However, the diversity of the structures of AGEs makes detection of these compounds more difficult. The aim of this study was to test a new method of AGE identification based on isotope (13)C labeling. The model protein (hen egg lysozyme) was modified with an equimolar mixture of [(12)C(6)]glucose and [(13)C(6)]glucose and then subjected to reduction of the disulfide bridges followed by tryptic hydrolysis. The digest obtained was analyzed by LC-MS. The glycation products were identified on the basis of characteristic isotopic patterns resulting from the use of isotopically labeled glucose. This method allowed identification of 38 early Maillard reaction products and five different structures of the end glycation products. This isotopic labeling technique combined with LC-MS is a sensitive method for identification of advanced glycation end products even if their chemical structure is unknown. Copyright © 2012 Elsevier Inc. All rights reserved.

Speciated Elemental and Isotopic Characterization of Atmospheric Aerosols - Recent Advances

NASA Astrophysics Data System (ADS)

Shafer, M.; Majestic, B.; Schauer, J.

2007-12-01

Detailed elemental, isotopic, and chemical speciation analysis of aerosol particulate matter (PM) can provide valuable information on PM sources, atmospheric processing, and climate forcing. Certain PM sources may best be resolved using trace metal signatures, and elemental and isotopic fingerprints can supplement and enhance molecular maker analysis of PM for source apportionment modeling. In the search for toxicologically relevant components of PM, health studies are increasingly demanding more comprehensive characterization schemes. It is also clear that total metal analysis is at best a poor surrogate for the bioavailable component, and analytical techniques that address the labile component or specific chemical species are needed. Recent sampling and analytical developments advanced by the project team have facilitated comprehensive characterization of even very small masses of atmospheric PM. Historically; this level of detail was rarely achieved due to limitations in analytical sensitivity and a lack of awareness concerning the potential for contamination. These advances have enabled the coupling of advanced chemical characterization to vital field sampling approaches that typically supply only very limited PM mass; e.g. (1) particle size-resolved sampling; (2) personal sampler collections; and (3) fine temporal scale sampling. The analytical tools that our research group is applying include: (1) sector field (high-resolution-HR) ICP-MS, (2) liquid waveguide long-path spectrophotometry (LWG-LPS), and (3) synchrotron x-ray absorption spectroscopy (sXAS). When coupled with an efficient and validated solubilization method, the HR-ICP-MS can provide quantitative elemental information on over 50 elements in microgram quantities of PM. The high mass resolution and enhanced signal-to-noise of HR-ICP-MS significantly advance data quality and quantity over that possible with traditional quadrupole ICP-MS. The LWG-LPS system enables an assessment of the soluble

Hydrogen isotope separation

DOEpatents

Bartlit, John R.; Denton, William H.; Sherman, Robert H.

1982-01-01

A system of four cryogenic fractional distillation columns interlinked with two equilibrators for separating a DT and hydrogen feed stream into four product streams, consisting of a stream of high purity D.sub.2, DT, T.sub.2, and a tritium-free stream of HD for waste disposal.

Hydrogen isotope separation

DOEpatents

Bartlit, J.R.; Denton, W.H.; Sherman, R.H.

Disclosed is a system of four cryogenic fractional distillation columns interlinked with two equilibrators for separating a DT and hydrogen feed stream into four product streams, consisting of a stream of high purity D/sub 2/, DT, T/sub 2/, and a tritium-free stream of HD for waste disposal.

A Reverse Osmosis System for an Advanced Separation Process Laboratory.

ERIC Educational Resources Information Center

Slater, C. S.; Paccione, J. D.

1987-01-01

Focuses on the development of a pilot unit for use in an advanced separations process laboratory in an effort to develop experiments on such processes as reverse osmosis, ultrafiltration, adsorption, and chromatography. Discusses reverse osmosis principles, the experimental system design, and some experimental studies. (TW)

Atomic and Molecular Beam Scattering: Characterizing Structure and Dynamics of Hybrid Organic-Semiconductor Interfaces and Introducing Novel Isotope Separation Techniques

NASA Astrophysics Data System (ADS)

Nihill, Kevin John

This thesis details a range of experiments and techniques that use the scattering of atomic beams from surfaces to both characterize a variety of interfaces and harness mass-specific scattering conditions to separate and enrich isotopic components in a mixture of gases. Helium atom scattering has been used to characterize the surface structure and vibrational dynamics of methyl-terminated Ge(111), thereby elucidating the effects of organic termination on a rigid semiconductor interface. Helium atom scattering was employed as a surface-sensitive, non-destructive probe of the surface. By means of elastic gas-surface diffraction, this technique is capable of providing measurements of atomic spacing, step height, average atomic displacement as a function of surface temperature, gas-surface potential well depth, and surface Debye temperature. Inelastic time-of-flight studies provide highly resolved energy exchange measurements between helium atoms and collective lattice vibrations, or phonons; a collection of these measurements across a range of incident kinematic parameters allowed for a thorough mapping of low-energy phonons (e.g., the Rayleigh wave) across the surface Brillouin zone and subsequent comparison with complementary theoretical calculations. The scattering of molecular beams - here, hydrogen and deuterium from methyl-terminated Si(111) - enables the measurement of the anisotropy of the gas-surface interaction potential through rotationally inelastic diffraction (RID), whereby incident atoms can exchange internal energy between translational and rotational modes and diffract into unique angular channels as a result. The probability of rotational excitations as a function of incident energy and angle were measured and compared with electronic structure and scattering calculations to provide insight into the gas-surface interaction potential and hence the surface charge density distribution, revealing important details regarding the interaction of H2 with an

Advances in stable isotope assisted labeling strategies with information science.

PubMed

Kigawa, Takanori

2017-08-15

Stable-isotope (SI) labeling of proteins is an essential technique to investigate their structures, interactions or dynamics by nuclear magnetic resonance (NMR) spectroscopy. The assignment of the main-chain signals, which is the fundamental first step in these analyses, is usually achieved by a sequential assignment method based on triple resonance experiments. Independently of the triple resonance experiment-based sequential assignment, amino acid-selective SI labeling is beneficial for discriminating the amino acid type of each signal; therefore, it is especially useful for the signal assignment of difficult targets. Various combinatorial selective labeling schemes have been developed as more sophisticated labeling strategies. In these strategies, amino acids are represented by combinations of SI labeled samples, rather than simply assigning one amino acid to one SI labeled sample as in the case of conventional amino acid-selective labeling. These strategies have proven to be useful for NMR analyses of difficult proteins, such as those in large complex systems, in living cells, attached or integrated into membranes, or with poor solubility. In this review, recent advances in stable isotope assisted labeling strategies will be discussed. Copyright © 2017 Elsevier Inc. All rights reserved.

Mercury Stable Isotopic Composition of Monomethylmercury in Estuarine Sediments and Pure Cultures of Mercury Methylating Bacteria

NASA Astrophysics Data System (ADS)

Janssen, S.; Johnson, M. W.; Barkay, T.; Blum, J. D.; Reinfelder, J. R.

2014-12-01

Tracking monomethylmercury (MeHg) from its source in soils and sediments through various environmental compartments and transformations is critical to understanding its accumulation in aquatic and terrestrial food webs. Advances in the field of mercury (Hg) stable isotopes have allowed for the tracking of discrete Hg sources and the examination of photochemical and bacterial transformations. Despite analytical advances, measuring the Hg stable isotopic signature of MeHg in environmental samples or laboratory experiments remains challenging due to difficulties in the quantitative separation of MeHg from complex matrices with high concentrations of inorganic Hg. To address these challenges, we have developed a MeHg isolation method for sediments and bacterial cultures which involves separation by gas chromatography. The MeHg eluting from the GC is passed through a pyrolysis column and purged onto a gold amalgam trap which is then desorbed into a final oxidizing solution. A MeHg reference standard carried through our separation process retained its isotopic composition within 0.02 ‰ for δ202Hg, and for native estuarine sediments, MeHg recoveries were 80% to 100%. For sediment samples from the Hackensack and Passaic Rivers (New Jersey, USA), δ202Hg values for MeHg varied from -1.2 to +0.58 ‰ (relative to SRM 3133) and for individual samples were significantly different from that of total Hg (-0.38 ± 0.06 ‰). No mass independent fractionation was observed in MeHg or total Hg from these sediments. Pure cultures of Geobacter sulfurreducens, grown under fermentative conditions showed preferential enrichment of lighter isotopes (lower δ202Hg) during Hg methylation. The Hg stable isotope signatures of MeHg in sediments and laboratory methylation experiments will be discussed in the context of the formation and degradation of MeHg in the environment and the bioaccumulation of MeHg in estuarine food webs.

Meteoritic Sulfur Isotopic Analysis

NASA Technical Reports Server (NTRS)

Thiemens, Mark H.

1996-01-01

Funds were requested to continue our program in meteoritic sulfur isotopic analysis. We have recently detected a potential nucleosynthetic sulfur isotopic anomaly. We will search for potential carriers. The documentation of bulk systematics and the possible relation to nebular chemistry and oxygen isotopes will be explored. Analytical techniques for delta(sup 33), delta(sup 34)S, delta(sup 36)S isotopic analysis were improved. Analysis of sub milligram samples is now possible. A possible relation between sulfur isotopes and oxygen was detected, with similar group systematics noted, particularly in the case of aubrites, ureilites and entstatite chondrites. A possible nucleosynthetic excess S-33 has been noted in bulk ureilites and an oldhamite separate from Norton County. High energy proton (approximately 1 GeV) bombardments of iron foils were done to experimentally determine S-33, S-36 spallogenic yields for quantitation of isotopic measurements in iron meteorites. Techniques for measurement of mineral separates were perfected and an analysis program initiated. The systematic behavior of bulk sulfur isotopes will continue to be explored.

[Advances of poly (ionic liquid) materials in separation science].

PubMed

Liu, Cuicui; Guo, Ting; Su, Rina; Gu, Yuchen; Deng, Qiliang

2015-11-01

Ionic liquids, as novel ionization reagents, possess beneficial characteristics including good solubility, conductivity, thermal stability, biocompatibility, low volatility and non-flammability. Ionic liquids are attracting a mass of attention of analytical chemists. Poly (ionic liquid) materials have common performances of ionic liquids and polymers, and have been successfully applied in separation science area. In this paper, we discuss the interaction mechanisms between the poly(ionic liquid) materials and analytes including hydrophobic/hydrophilic interactions, hydrogen bond, ion exchange, π-π stacking and electrostatic interactions, and summarize the application advances of the poly(ionic liquid) materials in solid phase extraction, chromatographic separation and capillary electrophoresis. At last, we describe the future prospect of poly(ionic liquid) materials.

Glacier advance during Marine Isotope Stage 11 in the McMurdo Dry Valleys of Antarctica

PubMed Central

Swanger, Kate M.; Lamp, Jennifer L.; Winckler, Gisela; Schaefer, Joerg M.; Marchant, David R.

2017-01-01

We mapped six distinct glacial moraines alongside Stocking Glacier in the McMurdo Dry Valleys, Antarctica. Stocking Glacier is one of several alpine glaciers in the Dry Valleys fringed by multiple cold-based drop moraines. To determine the age of the outermost moraine, we collected 10 boulders of Ferrar Dolerite along the crest of the moraine and analyzed mineral separates of pyroxene for cosmogenic 3He. On the basis of these measurements, the exposure age for the outermost moraine is 391 ± 35 ka. This represents the first documented advance of alpine glacier ice in the Dry Valleys during Marine Isotope Stage (MIS) 11. At this time, Stocking Glacier was ~20–30% larger than today. The cause of ice expansion is uncertain, but most likely it is related to increased atmospheric temperature and precipitation, associated with reduced ice extent in the nearby Ross Embayment. The data suggest complex local environmental response to warm climates in Antarctica and have implications for glacial response to Holocene warming. The study also demonstrates the potential for using alpine glacier chronologies in the Transantarctic Mountains as proxies for retreat of grounded glacier ice in the Ross Embayment. PMID:28139676

Isotopic separation of snowmelt runoff during an artificial rain-on-snow event

NASA Astrophysics Data System (ADS)

Juras, Roman; Pavlasek, Jirka; Šanda, Martin; Jankovec, Jakub; Linda, Miloslav

2013-04-01

Rain-on-snow events are common phenomenon in the climate conditions of central Europe, mainly during the spring snowmelt period. These events can cause serious floods in areas with seasonal snow. The snowpack hit by rain is able to store a fraction of rain water, but runoff caused by additional snowmelt also increases. Assessment of the rainwater ratio contributing to the outflow from the snowpack is therefore critical for discharge modelling. A rainfall simulator and water enriched by deuterium were used for the study of rainwater behaviour during an artificial rain-on-snow event. An area of 1 m2 of the snow sample, which was 1.2 m deep, consisting of ripped coarse-grained snow, was sprayed during the experiment with deuterium enriched water. The outflow from the snowpack was measured and samples of outflow water were collected. The isotopic content of deuterium was further analyzed from these samples by means of laser spectroscopy for the purpose of hydrograph separation. The concentration of deuterium in snow before and after the experiment was also investigated. The deuterium enriched water above the natural concentration of deuterium in snowpack was detected in the outflow in 7th minute from start of spraying, but the significant increase of deuterium concentration in outflow was observed in 19th minute. The isotopic hydrograph separation estimated, that deuterium enriched rainwater became the major part (> 50% volumetric) of the outflow in 28th minute. The culmination of the outflow (1.23 l min-1) as well as deuterium enriched rainwater fraction (63.5%) in it occurred in 63th minute, i.e. right after the end of spraying. In total, 72.7 l of deuterium enriched water was sprayed on the snowpack in 62 minutes. Total volume of outflow (after 12.3 hours) water was 97.4 l, which contained 48.3 l of deuterium enriched water (i.e. 49.6 %) and 49.1 l (50.4 %) of the melted snowpack. The volume of 24.4 l of deuterium enriched spray-water was stored in the snowpack. The

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.

Conventional and Advanced Separations in Mass Spectrometry-Based Metabolomics: Methodologies and Applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heyman, Heino M.; Zhang, Xing; Tang, Keqi

2016-02-16

Metabolomics is the quantitative analysis of all metabolites in a given sample. Due to the chemical complexity of the metabolome, optimal separations are required for comprehensive identification and quantification of sample constituents. This chapter provides an overview of both conventional and advanced separations methods in practice for reducing the complexity of metabolite extracts delivered to the mass spectrometer detector, and covers gas chromatography (GC), liquid chromatography (LC), capillary electrophoresis (CE), supercritical fluid chromatography (SFC) and ion mobility spectrometry (IMS) separation techniques coupled with mass spectrometry (MS) as both uni-dimensional and as multi-dimensional approaches.

Crosscutting Technology Development at the Center for Advanced Separation Technologies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Christopher E. Hull

2006-09-30

This Technical Progress Report describes progress made on the twenty nine subprojects awarded in the second year of Cooperative Agreement DE-FC26-02NT41607: Crosscutting Technology Development at the Center for Advanced Separation Technologies. This work is summarized in the body of the main report: the individual sub-project Technical Progress Reports are attached as Appendices.

CROSSCUTTING TECHNOLOGY DEVELOPMENT AT THE CENTER FOR ADVANCED SEPARATION TECHNOLOGIES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Christopher E. Hull

2006-05-15

This Technical Progress Report describes progress made on the twenty nine subprojects awarded in the second year of Cooperative Agreement DE-FC26-02NT41607: Crosscutting Technology Development at the Center for Advanced Separation Technologies. This work is summarized in the body of the main report: the individual sub-project Technical Progress Reports are attached as Appendices.

Modified ion exchange separation for tungsten isotopic measurements from kimberlite samples using multi-collector inductively coupled plasma mass spectrometry.

PubMed

Sahoo, Yu Vin; Nakai, Shun'ichi; Ali, Arshad

2006-03-01

Tungsten isotope composition of a sample of deep-seated rock can record the influence of core-mantle interaction of the parent magma. Samples of kimberlite, which is known as a carrier of diamond, from the deep mantle might exhibit effects of core-mantle interaction. Although tungsten isotope anomaly was reported for kimberlites from South Africa, a subsequent investigation did not verify the anomaly. The magnesium-rich and calcium-rich chemical composition of kimberlite might engender difficulty during chemical separation of tungsten for isotope analyses. This paper presents a simple, one-step anion exchange technique for precise and accurate determination of tungsten isotopes in kimberlites using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Large quantities of Ca and Mg in kimberlite samples were precipitated and removed with aqueous H(2)SO(4). Highly pure fractions of tungsten for isotopic measurements were obtained following an anion exchange chromatographic procedure involving mixed acids. That procedure enabled efficient removal of high field strength elements (HFSE), such as Hf, Zr and Ti, which are small ions that carry strong charges and develop intense electrostatic fields. The tungsten yields were 85%-95%. Advantages of this system include less time and less use of reagents. Precise and accurate isotopic measurements are possible using fractions of tungsten that are obtained using this method. The accuracy and precision of these measurements were confirmed using various silicate standard rock samples, JB-2, JB-3 and AGV-1.

Hydrogen isotope separation from water

DOEpatents

Jensen, R.J.

1975-09-01

A process for separating tritium from tritium-containing water or deuterium enrichment from water is described. The process involves selective, laser-induced two-photon excitation and photodissociation of those water molecules containing deuterium or tritium followed by immediate reaction of the photodissociation products with a scavenger gas which does not substantially absorb the laser light. The reaction products are then separated from the undissociated water. (auth)

Integrated Extraction Chromatographic Separation of the Lithophile Elements Involved in Long-Lived Radiogenic Isotope Systems (Rb-Sr, U-Th-Pb, Sm-Nd, La-Ce, and Lu-Hf) Useful in Geochemical and Environmental Sciences.

PubMed

Pin, Christian; Gannoun, Abdelmouhcine

2017-02-21

A fast and efficient sample preparation method in view of isotope ratio measurements is described, allowing the separation of 11 elements involved, either as "parent" or as "daughter" isotopes, in six radiogenic isotope systems used as chronometers and tracers in earth, planetary, and environmental sciences. The protocol is based on small extraction chromatographic columns, used either alone or in tandem, through which a single nitric acid solution is passed, without any intervening evaporation step. The columns use commercially available extraction resins (Sr resin, TRU resin, Ln resin, RE resin, and again Ln resin for isolating Sr and Pb, LREE then La-Ce-Nd-Sm, Lu(Yb), and Hf, Th, and U, respectively) along with an additional, in-house prepared resin for separating Rb. A simplified scheme is proposed for samples requiring the separation of Sr, Pb, Nd, and Hf only. Adverse effects of troublesome major elements (Fe 3+ , Ti) are circumvented by masking with ascorbic acid and hydrofluoric acid, respectively. Typical recoveries in the 85-95% range are achieved, with procedural blanks of 10-100 pg, negligible with regard to the amounts of analytes processed. The fractions separated are suitable for high precision isotope ratio measurements by TIMS or MC-ICP-MS, as demonstrated by the repeat analyses of several international reference materials of basaltic composition for 87 Sr/ 86 Sr, 208,207,206 Pb/ 204 Pb, 143 Nd/ 144 Nd, 176 Hf/ 177 Hf, and 230 Th/ 232 Th. Concentration data could be obtained by spiking and equilibrating the sample with appropriate isotopic tracers before the onset of the separation process and, finally, measuring the isotope ratios modified by the isotope dilution process.

Separation of Platinum from Palladium and Iridium in Iron Meteorites and Accurate High-Precision Determination of Platinum Isotopes by Multi-Collector ICP-MS.

PubMed

Hunt, Alison C; Ek, Mattias; Schönbächler, Maria

2017-12-01

This study presents a new measurement procedure for the isolation of Pt from iron meteorite samples. The method also allows for the separation of Pd from the same sample aliquot. The separation entails a two-stage anion-exchange procedure. In the first stage, Pt and Pd are separated from each other and from major matrix constituents including Fe and Ni. In the second stage, Ir is reduced with ascorbic acid and eluted from the column before Pt collection. Platinum yields for the total procedure were typically 50-70%. After purification, high-precision Pt isotope determinations were performed by multi-collector ICP-MS. The precision of the new method was assessed using the IIAB iron meteorite North Chile. Replicate analyses of multiple digestions of this material yielded an intermediate precision for the measurement results of 0.73 for ε 192 Pt, 0.15 for ε 194 Pt and 0.09 for ε 196 Pt (2 standard deviations). The NIST SRM 3140 Pt solution reference material was passed through the measurement procedure and yielded an isotopic composition that is identical to the unprocessed Pt reference material. This indicates that the new technique is unbiased within the limit of the estimated uncertainties. Data for three iron meteorites support that Pt isotope variations in these samples are due to exposure to galactic cosmic rays in space.

Crosscutting Technology Development at the Center for Advanced Separation Technologies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Christopher Hull

2009-10-31

The U.S. is the largest producer of mining products in the world. In 2003, U.S. mining operations produced $57 billion worth of raw materials that contributed a total of $564 billion to the nation's wealth. Despite these contributions, the mining industry has not been well supported with research and development funds as compared to mining industries in other countries. To overcome this problem, the Center for Advanced Separation Technologies (CAST) was established to develop technologies that can be used by the U.S. mining industry to create new products, reduce production costs, and meet environmental regulations. Originally set up by Virginiamore » Tech and West Virginia University, this endeavor has been expanded into a seven-university consortium -- Virginia Tech, West Virginia University, University of Kentucky, University of Utah, Montana Tech, New Mexico Tech and University of Nevada, Reno - that is supported through U.S. DOE Cooperative Agreement No. DE-FC26-02NT41607: Crosscutting Technology Development at the Center for Advanced Separation Technologies. Much of the research to be conducted with Cooperative Agreement funds will be longer-term, high-risk, basic research and will be carried out in five broad areas: (1) Solid-solid separation; (2) Solid-liquid separation; (3) Chemical/biological extraction; (4) Modeling and control; and (5) Environmental control. Distribution of funds is handled via competitive solicitation of research proposals through Site Coordinators at the seven member universities. These were first reviewed and ranked by a group of technical reviewers (selected primarily from industry). Based on these reviews, and an assessment of overall program requirements, the CAST Technical Committee made an initial selection/ranking of proposals and forwarded these to the DOE/NETL Project Officer for final review and approval. The successful projects are listed by category, along with brief abstracts of their aims and objectives.« less

Development of Advanced Nuclide Separation and Recovery Methods using Ion-Exchanhge Techniques in Nuclear Backend

NASA Astrophysics Data System (ADS)

Miura, Hitoshi

The development of compact separation and recovery methods using selective ion-exchange techniques is very important for the reprocessing and high-level liquid wastes (HLLWs) treatment in the nuclear backend field. The selective nuclide separation techniques are effective for the volume reduction of wastes and the utilization of valuable nuclides, and expected for the construction of advanced nuclear fuel cycle system and the rationalization of waste treatment. In order to accomplish the selective nuclide separation, the design and synthesis of novel adsorbents are essential for the development of compact and precise separation processes. The present paper deals with the preparation of highly functional and selective hybrid microcapsules enclosing nano-adsorbents in the alginate gel polymer matrices by sol-gel methods, their characterization and the clarification of selective adsorption properties by batch and column methods. The selective separation of Cs, Pd and Re in real HLLW was further accomplished by using novel microcapsules, and an advanced nuclide separation system was proposed by the combination of selective processes using microcapsules.

Recent advances in stable isotope labeling based techniques for proteome relative quantification.

PubMed

Zhou, Yuan; Shan, Yichu; Zhang, Lihua; Zhang, Yukui

2014-10-24

The large scale relative quantification of all proteins expressed in biological samples under different states is of great importance for discovering proteins with important biological functions, as well as screening disease related biomarkers and drug targets. Therefore, the accurate quantification of proteins at proteome level has become one of the key issues in protein science. Herein, the recent advances in stable isotope labeling based techniques for proteome relative quantification were reviewed, from the aspects of metabolic labeling, chemical labeling and enzyme-catalyzed labeling. Furthermore, the future research direction in this field was prospected. Copyright © 2014 Elsevier B.V. All rights reserved.

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.

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.

Development of an on-line flow injection Sr/matrix separation method for accurate, high-throughput determination of Sr isotope ratios by multiple collector-inductively coupled plasma-mass spectrometry.

PubMed

Galler, Patrick; Limbeck, Andreas; Boulyga, Sergei F; Stingeder, Gerhard; Hirata, Takafumi; Prohaska, Thomas

2007-07-01

This work introduces a newly developed on-line flow injection (FI) Sr/Rb separation method as an alternative to the common, manual Sr/matrix batch separation procedure, since total analysis time is often limited by sample preparation despite the fast rate of data acquisition possible by inductively coupled plasma-mass spectrometers (ICPMS). Separation columns containing approximately 100 muL of Sr-specific resin were used for on-line FI Sr/matrix separation with subsequent determination of (87)Sr/(86)Sr isotope ratios by multiple collector ICPMS. The occurrence of memory effects exhibited by the Sr-specific resin, a major restriction to the repetitive use of this costly material, could successfully be overcome. The method was fully validated by means of certified reference materials. A set of two biological and six geological Sr- and Rb-bearing samples was successfully characterized for its (87)Sr/(86)Sr isotope ratios with precisions of 0.01-0.04% 2 RSD (n = 5-10). Based on our measurements we suggest (87)Sr/(86)Sr isotope ratios of 0.713 15 +/- 0.000 16 (2 SD) and 0.709 31 +/- 0.000 06 (2 SD) for the NIST SRM 1400 bone ash and the NIST SRM 1486 bone meal, respectively. Measured (87)Sr/(86)Sr isotope ratios for five basalt samples are in excellent agreement with published data with deviations from the published value ranging from 0 to 0.03%. A mica sample with a Rb/Sr ratio of approximately 1 was successfully characterized for its (87)Sr/(86)Sr isotope signature to be 0.718 24 +/- 0.000 29 (2 SD) by the proposed method. Synthetic samples with Rb/Sr ratios of up to 10/1 could successfully be measured without significant interferences on mass 87, which would otherwise bias the accuracy and uncertainty of the obtained data.

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.

Late metal-silicate separation on the IAB parent asteroid: Constraints from combined W and Pt isotopes and thermal modelling

NASA Astrophysics Data System (ADS)

Hunt, Alison C.; Cook, David L.; Lichtenberg, Tim; Reger, Philip M.; Ek, Mattias; Golabek, Gregor J.; Schönbächler, Maria

2018-01-01

The short-lived 182Hf-182W decay system is a powerful chronometer for constraining the timing of metal-silicate separation and core formation in planetesimals and planets. Neutron capture effects on W isotopes, however, significantly hamper the application of this tool. In order to correct for neutron capture effects, Pt isotopes have emerged as a reliable in-situ neutron dosimeter. This study applies this method to IAB iron meteorites, in order to constrain the timing of metal segregation on the IAB parent body. The ε182W values obtained for the IAB iron meteorites range from -3.61 ± 0.10 to -2.73 ± 0.09. Correlating εiPt with ε182W data yields a pre-neutron capture ε182W of -2.90 ± 0.06. This corresponds to a metal-silicate separation age of 6.0 ± 0.8 Ma after CAI for the IAB parent body, and is interpreted to represent a body-wide melting event. Later, between 10 and 14 Ma after CAI, an impact led to a catastrophic break-up and subsequent reassembly of the parent body. Thermal models of the interior evolution that are consistent with these estimates suggest that the IAB parent body underwent metal-silicate separation as a result of internal heating by short-lived radionuclides and accreted at around 1.4 ± 0.1 Ma after CAIs with a radius of greater than 60 km.

Method for sequential injection of liquid samples for radioisotope separations

DOEpatents

Egorov, Oleg B.; Grate, Jay W.; Bray, Lane A.

2000-01-01

The present invention is a method of separating a short-lived daughter isotope from a longer lived parent isotope, with recovery of the parent isotope for further use. Using a system with a bi-directional pump and one or more valves, a solution of the parent isotope is processed to generate two separate solutions, one of which contains the daughter isotope, from which the parent has been removed with a high decontamination factor, and the other solution contains the recovered parent isotope. The process can be repeated on this solution of the parent isotope. The system with the fluid drive and one or more valves is controlled by a program on a microprocessor executing a series of steps to accomplish the operation. In one approach, the cow solution is passed through a separation medium that selectively retains the desired daughter isotope, while the parent isotope and the matrix pass through the medium. After washing this medium, the daughter is released from the separation medium using another solution. With the automated generator of the present invention, all solution handling steps necessary to perform a daughter/parent radionuclide separation, e.g. Bi-213 from Ac-225 "cow" solution, are performed in a consistent, enclosed, and remotely operated format. Operator exposure and spread of contamination are greatly minimized compared to the manual generator procedure described in U.S. patent application Ser. No. 08/789,973, now U.S. Pat. No. 5,749,042, herein incorporated by reference. Using 16 mCi of Ac-225 there was no detectable external contamination of the instrument components.

Method and apparatus for separation of heavy and tritiated water

DOEpatents

Lee, Myung W.

2001-01-01

The present invention is a bi-thermal membrane process for separating and recovering hydrogen isotopes from a fluid containing hydrogen isotopes, such as water and hydrogen gas. The process in accordance with the present invention provides counter-current cold and hot streams of the fluid separated with a thermally insulating and chemically transparent proton exchange membrane (PEM). The two streams exchange hydrogen isotopes through the membrane: the heavier isotopes migrate into the cold stream, while the lighter isotopes migrate into the hot stream. The heavy and light isotopes are continuously withdrawn from the cold and hot streams respectively.

Gaseous isotope separation using solar wind phenomena.

PubMed

Wang, C G

1980-12-01

A large evacuated drum-like chamber fitted with supersonic nozzles in the center, with the chamber and the nozzles corotating, can separate gaseous fluids according to their molecular weights. The principle of separation is essentially the same as that of the solar wind propagation, in which components of the plasma fluid are separated due to their difference in the time-of-flight. The process can inherently be very efficient, serving as a pump as well as a separator, and producing well over 10(5) separative work units (kg/year) for the hydrogen/deuterium mixture at high-velocity flows.

A superhydrophobic copper mesh as an advanced platform for oil-water separation

NASA Astrophysics Data System (ADS)

Ren, Guina; Song, Yuanming; Li, Xiangming; Zhou, Yanli; Zhang, Zhaozhu; Zhu, Xiaotao

2018-01-01

Improving the separation efficiency and simplifying the separation process would be highly desired for oil-water separation yet still challenging. Herein, to address this challenge, we fabricated a superhydrophobic copper mesh by an immersion process and exploited it as an advanced platform for oil-water separation. To realize oil-water separation efficiently, the obtained mesh was enfolded directly to form a boat-like device, and it could also be mounted on an open end of a glass barrel to form the oil skimmer device. For these devices, they can collect the floating oils through the pores of the copper mesh while repelling water completely, and the oil collection efficiency is up to 99.5%. Oils collected in the devices can be easily sucked out into a container for storing, without requiring mechanical handing for recycling. Importantly, the miniature boat and the oil skimmer devices can retain their enhanced oil collection efficiency even after 10 cycles of oil-water separation. Moreover, exploiting its superhydrophobicity under oil, the obtained copper mesh was demonstrated as a novel platform to remove tiny water droplets from oil.

Intramolecular carbon and nitrogen isotope analysis by quantitative dry fragmentation of the phenylurea herbicide isoproturon in a combined injector/capillary reactor prior to GC separation.

PubMed

Penning, Holger; Elsner, Martin

2007-11-01

Potentially, compound-specific isotope analysis may provide unique information on source and fate of pesticides in natural systems. Yet for isotope analysis, LC-based methods that are based on the use of organic solvents often cannot be used and GC-based analysis is frequently not possible due to thermolability of the analyte. A typical example of a compound with such properties is isoproturon (3-(4-isopropylphenyl)-1,1-dimethylurea), belonging to the worldwide extensively used phenylurea herbicides. To make isoproturon accessible to carbon and nitrogen isotope analysis, we developed a GC-based method during which isoproturon was quantitatively fragmented to dimethylamine and 4-isopropylphenylisocyanate. Fragmentation occurred only partially in the injector but was mainly achieved on a heated capillary column. The fragments were then chromatographically separated and individually measured by isotope ratio mass spectrometry. The reliability of the method was tested in hydrolysis experiments with three isotopically different batches of isoproturon. For all three products, the same isotope fractionation factors were observed during conversion and the difference in isotope composition between the batches was preserved. This study demonstrates that fragmentation of phenylurea herbicides does not only make them accessible to isotope analysis but even enables determination of intramolecular isotope fractionation.

Advanced flight hardware for organic separations using aqueous two-phase partitioning

NASA Astrophysics Data System (ADS)

Deuser, Mark S.; Vellinger, John C.; Weber, John T.

1996-03-01

Separation of cells and cell components is the limiting factor in many biomedical research and pharmaceutical development processes. Aqueous Two-Phase Partitioning (ATPP) is a unique separation technique which allows purification and classification of biological materials. SHOT has employed the ATPP process in separation equipment developed for both space and ground applications. Initial equipment development and research focused on the ORganic SEParation (ORSEP) space flight experiments that were performed on suborbital rockets and the shuttle. ADvanced SEParations (ADSEP) technology was developed as the next generation of ORSEP equipment through a NASA Small Business Innovation Research (SBIR) contract. Under the SBIR contract, a marketing study was conducted, indicating a growing commercial market exists among biotechnology firms for ADSEP equipment and associated flight research and development services. SHOT is preparing to begin manufacturing and marketing laboratory versions of the ADSEP hardware for the ground-based market. In addition, through a self-financed SBIR Phase III effort, SHOT is fabricating and integrating the ADSEP flight hardware for a commercially-driven SPACEHAB 04 experiment that will be the initial step in marketing space separations services. The ADSEP ground-based and microgravity research is expected to play a vital role in developing important new biomedical and pharmaceutical products.

Advanced Separators for Lithium-Ion and Lithium-Sulfur Batteries: A Review of Recent Progress.

PubMed

Xiang, Yinyu; Li, Junsheng; Lei, Jiaheng; Liu, Dan; Xie, Zhizhong; Qu, Deyu; Li, Ke; Deng, Tengfei; Tang, Haolin

2016-11-09

Li-ion and Li-S batteries find enormous applications in different fields, such as electric vehicles and portable electronics. A separator is an indispensable part of the battery design, which functions as a physical barrier for the electrode as well as an electrolyte reservoir for ionic transport. The properties of the separators directly influence the performance of the batteries. Traditional polyolefin separators showed low thermal stability, poor wettability toward the electrolyte, and inadequate barrier properties to polysulfides. To improve the performance and durability of Li-ion and Li-S batteries, development of advanced separators is required. In this review, we summarize recent progress on the fabrication and application of novel separators, including the functionalized polyolefin separator, polymeric separator, and ceramic separator, for Li-ion and Li-S batteries. The characteristics, advantages, and limitations of these separators are discussed. A brief outlook for the future directions of the research in the separators is also provided. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Tracking millennial-scale Holocene glacial advance and retreat using osmium isotopes: Insights from the Greenland ice sheet

USGS Publications Warehouse

Rooney, Alan D.; Selby, David; Llyod, Jeremy M.; Roberts, David H.; Luckge, Andreas; Sageman, Bradley B.; Prouty, Nancy G.

2016-01-01

High-resolution Os isotope stratigraphy can aid in reconstructing Pleistocene ice sheet fluctuation and elucidating the role of local and regional weathering fluxes on the marine Os residence time. This paper presents new Os isotope data from ocean cores adjacent to the West Greenland ice sheet that have excellent chronological controls. Cores MSM-520 and DA00-06 represent distal to proximal sites adjacent to two West Greenland ice streams. Core MSM-520 has a steadily decreasing Os signal over the last 10 kyr (187Os/188Os = 1.35–0.81). In contrast, Os isotopes from core DA00-06 (proximal to the calving front of Jakobshavn Isbræ) highlight four stages of ice stream retreat and advance over the past 10 kyr (187Os/188Os = 2.31; 1.68; 2.09; 1.47). Our high-resolution chemostratigraphic records provide vital benchmarks for ice-sheet modelers as we attempt to better constrain the future response of major ice sheets to climate change. Variations in Os isotope composition from sediment and macro-algae (seaweed) sourced from regional and global settings serve to emphasize the overwhelming effect weathering sources have on seawater Os isotope composition. Further, these findings demonstrate that the residence time of Os is shorter than previous estimates of ∼104 yr.

Radiogenic Isotopes As Paleoceanographic Tracers in Deep-Sea Corals: Advances in TIMS Measurements of Pb Isotopes and Application to Southern Ocean Corals

NASA Astrophysics Data System (ADS)

Wilson, D. J.; van de Flierdt, T.; Bridgestock, L. J.; Paul, M.; Rehkamper, M.; Robinson, L. F.; Adkins, J. F.

2014-12-01

Deep-sea corals have emerged as a valuable archive of deep ocean paleoceanographic change, with uranium-series dating providing absolute ages and the potential for centennial resolution. In combination with measurements of radiocarbon, neodymium isotopes and clumped isotopes, this archive has recently been exploited to reconstruct changes in ventilation, water mass sourcing and temperature in relation to millennial climate change. Lead (Pb) isotopes in both corals and seawater have also been used to track anthropogenic inputs through space and time and to trace transport pathways within the oceans. Better understanding of the oceanic Pb cycle is emerging from the GEOTRACES programme. However, while Pb isotopes have been widely used in environmental studies, their full potential as a (pre-anthropogenic) paleoceanographic tracer remains to be exploited. In deep-sea corals, challenges exist from low Pb concentrations in aragonite in comparison to secondary coatings, the potential for contamination, and the efficient elemental separation required for measurement by thermal ionisation mass spectrometry (TIMS). Here we discuss progress in measuring Pb isotopes in coral aragonite using a 207Pb-204Pb double spike on a ThermoFinnigan Triton TIMS. For a 2 ng NIST-981 Pb standard, the long term reproducibility (using 1011 Ω resistors) is ~1000 ppm (2 s.d.) on 206Pb/204Pb, 207Pb/204Pb and 208Pb/204Pb ratios. We now show that using a new 1012 Ω resistor to measure the small 204Pb beam improves the internal precision on these ratios from ~500 ppm (2 s.e.) to ~250 ppm (2 s.e.) and we envisage a potential improvement in the long term reproducibility as a consequence. We further assess the internal precision and external reproducibility of our method using a BCR-2 rock standard and an in-house coral standard. Preliminary evidence on the application of this method to natural samples is derived from cleaning experiments and replication tests on deep-sea corals from the Southern

Isotopic separation of He-3/He-4 from solar wind gases evolved from the lunar regolith

NASA Astrophysics Data System (ADS)

Wilkes, William R.; Wittenberg, Layton J.

The potential benefits of He-3 when utilized in a nuclear fusion reactor to provide clean, safe electricity in the 21st century for the world's inhabitants has been documented. Unfortunately, He is scarce on earth. Large quantities of He-3, perhaps a million tons, are embedded in the lunar regolith, presumably implanted by the solar wind together with other elements, notably He-4, H, C, and N. Several studies have suggested processing the lunar regolith and recovering these valuable solar wind gases. Once released, these gases can be separated for use. The separation of helium isotopes is described in this paper. He-3 constitutes only 400 at. ppm of lunar He, too dilute to separate economically by distillation alone. A 'superfluid' separator is being considered to preconcentrate the He-3. The superfluid separator consists of a porous filter in a tube maintained at a temperature of 2.17 K or less. Although the He-4, which is superfluid below 2.17 K, flows readily through the filter, the He is blocked by the filter, and becomes enriched at the feed end. He can be enriched to about 10 percent in such a system. The enriched product from the superfluid separation serves as a feed to a distillation apparatus operating at a pressure of 9 kPa, with a boiler temperature of 2.4 K, and a condenser temperature of 1.6 K. Under constant flow conditions, a 99.9 percent enriched He product can be produced in this apparatus. The heat rejection load of the refrigeration equipment necessary to cool the separation operations would be conducted during the lunar nights.

Mass dependence of calcium isotope fractionations in crown-ether resin chromatography.

PubMed

Fujii, Yasuhiko; Nomura, Masao; Kaneshiki, Tositaka; Sakuma, Yoichi; Suzuki, Tatsuya; Umehara, Saori; Kishimoto, Tadahumi

2010-06-01

Benzo 18-crown-6-ether resin was synthesised by the phenol condensation polymerisation process in porous silica beads, of which particle diameter was ca 60micro Calcium adsorption chromatography was performed with the synthesised resin packed in a glass column. The effluent was sampled in fractions, and the isotopic abundance ratios of (42)Ca, (43)Ca, (44)Ca, and (48)Ca against (40)Ca were measured by a thermo-ionisation mass spectrometer. The enrichment of heavier calcium isotopes was observed at the front boundary of calcium adsorption chromatogram. The mass dependence of mutual separation of calcium isotopes was analysed by using the three-isotope-plots method. The slopes of three-isotope-plots indicate the relative values of mutual separation coefficients for concerned isotopic pairs. The results have shown the normal mass dependence; isotope fractionation is proportional to the reduced mass difference, (M - M')/MM', where M and M' are masses of heavy and light isotope, respectively. The mass dependence clarifies that the isotope fractionations are originated from molecular vibration. The observed separation coefficient epsilon is 3.1x10(-3) for the pair of (40)Ca and (48)Ca. Productivity of enriched (48)Ca by crown-ether-resin was discussed as the function of the separation coefficient and the height equivalent to the theoretical plate.

Advancing an In situ Laser Spectrometer for Carbon Isotope Analyses in the Deep Ocean

NASA Astrophysics Data System (ADS)

Michel, A.; Wankel, S. D.; Kapit, J.; Girguis, P. R.

2016-02-01

Development of in situ chemical sensors is critical for improving our understanding of deep-ocean biogeochemistry and recent advances in chemical sensors are already expanding the breadth and depth of deep sea/seafloor exploration and research. Although initially developed for high sensitivity measurements of atmospheric gases, laser-based spectroscopic sensors are now being developed for research in the deep sea by incorporating the use of semi-permeable membranes. Here we present on recent deep-sea deployments of an in situ laser-based analyzer of carbon isotopes of methane (δ13CH4), highlighting several advances including a new capability for also measuring δ13C of DIC or CO2 by incorporating a second laser and an in line acidification module. A bubble trapping approach was designed and implemented for the collection and analysis of both CH4 and CO2 from deep-sea bubbles. The newly advanced laser spectrometer was deployed at both Kick `Em Jenny volcano off of the island of Grenada and in a brine pool in the western Gulf of Mexico ("The Jacuzzi of Despair") using the E/V Nautilus and the ROV Hercules. At Kick `Em Jenny, seafloor measurements were made of both emanating fluids and bubbles from within and around the crater - revealing high levels of magmatic CO2 with minor amounts of CH4 and hydrogen sulfide. At the brine pool, spot measurements and depth profile measurements into the brine pool were made for chemical mapping, revealing fluids that were saturated with respect to methane. New technologies such as the laser spectrometer will enable us to obtain high resolution and near real-time, in situ chemical and isotopic data and to make geochemical maps over a range of spatial and temporal scales.

A Critical Look at the Combined Use of Sulfur and Oxygen Isotopes to Study Microbial Metabolisms in Methane-Rich Environments

PubMed Central

Antler, Gilad; Pellerin, André

2018-01-01

Separating the contributions of anaerobic oxidation of methane and organoclastic sulfate reduction in the overall sedimentary sulfur cycle of marine sediments has benefited from advances in isotope biogeochemistry. Particularly, the coupling of sulfur and oxygen isotopes measured in the residual sulfate pool (δ18OSO4 vs. δ34SSO4). Yet, some important questions remain. Recent works have observed patterns that are inconsistent with previous interpretations. We differentiate the contributions of oxygen and sulfur isotopes to separating the anaerobic oxidation of methane and organoclastic sulfate reduction into three phases; first evidence from conventional high methane vs. low methane sites suggests a clear relationship between oxygen and sulfur isotopes in porewater and the metabolic process taking place. Second, evidence from pure cultures and organic matter rich sites with low levels of methane suggest the signatures of both processes overlap and cannot be differentiated. Third, we take a critical look at the use of oxygen and sulfur isotopes to differentiate metabolic processes (anaerobic oxidation of methane vs. organoclastic sulfate reduction). We identify that it is essential to develop a better understanding of the oxygen kinetic isotope effect, the degree of isotope exchange with sulfur intermediates as well as establishing their relationships with the cell-specific metabolic rates if we are to develop this proxy into a reliable tool to study the sulfur cycle in marine sediments and the geological record. PMID:29681890

Investigating the Relationship Between Soil Water Mobility and Stable Isotope Composition with Implications for the Ecohydrologic Separation Hypothesis

NASA Astrophysics Data System (ADS)

Shuler, J.; McNamara, J. P.; Benner, S. G.; Kohn, M. J.; Evans, S.

2017-12-01

The ecohydrologic separation (ES) hypothesis states that streams and plants return different soil water compartments to the atmosphere and that these compartments bear distinct isotopic compositions that can be used to infer soil water mobility. Recent studies have found isotopic evidence for ES in a variety of ecosystems, though interpretations of these data vary. ES investigations frequently suffer from low sampling frequencies as well as incomplete or missing soil moisture and matric potential data to support assumptions of soil water mobility. We sampled bulk soil water every 2-3 weeks in the upper 1 m of a hillslope profile from May 2016 to July 2017 in a semi-arid watershed outside Boise, ID. Twig samples of three plant species were also collected concurrently. Plant and soil water samples extracted via cryogenic vacuum distillation were analyzed for δ2H and δ18O composition. Soil moisture and soil matric potential sensors were installed at five and four depths in the profile, respectively. Shallow bulk soil water was progressively enriched in both isotopes over the growing season and plotted along a soil evaporation line in a plot of δ2H versus δ18O. Plant water during the growing season plotted below both the Local Meteoric Water Line and soil evaporation line. Plant water isotopic composition could not be traced to any source sampled in this study. Additionally, soil moisture and matric potential data revealed that soils were well-drained and that mobile soil water was unavailable throughout most of the growing season at the depths sampled. Soil water isotopic composition alone failed to predict mobility as observed in soil moisture and matric potential data. These results underscore the need for standard hydrologic definitions for the mobile and immobile compartments of soil water in future studies of the ES hypothesis and ecohydrologic processes in general.

Conformational effect of dicyclo-hexano-18-crown-6 on isotopic fractionation of zinc: DFT approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Boda, A.; Singha Deb, A. K.; Ali, Sk. M.

2014-04-24

Generalized gradient approximated BP86 density functional employing triple zeta valence plus polarization (TZVP) basis set has been used to compute the reduced partition function ratio and isotopic separation factor for zinc isotopes. The isotopic separation factor was found to be in good agreement with the experimental results. The isotopic separation factor was found to depend on the conformation of the crown ether ligand. The trans-trans conformation shows the highest fractionation compared to cis-cis conformer. The present theoretical results can thus be used to plan the isotope separation experiments.

Recent advances in capillary electrophoresis separation of monosaccharides, oligosaccharides, and polysaccharides.

PubMed

Mantovani, Veronica; Galeotti, Fabio; Maccari, Francesca; Volpi, Nicola

2018-01-01

This article illustrates the basis and applications of methodologies for the analysis of simple and complex carbohydrates by means of CE. After a description of the most common and novel approaches useful for the analysis and characterization of carbohydrates, this review covers the recent advances in CE separation of monosaccharides, oligosaccharides, and polysaccharides. Various CE techniques are also illustrated for the study of carbohydrates derived from complex glyco-derivatives such as glycoproteins and glycolipids, essential for biopharmaceutical and glycoproteomics applications as well as for biomarker detection. Most glycans have no significant UV absorption, and derivatization with fluorophore groups prior to separation usually results in higher sensitivity and an improved electrophoretic profile. We also discuss the recent applications and separations by CE of derivatized simple and more complex carbohydrates with different chromophoric active tags. Overall, this review aims to give an overview of the most recent state-of-the-art techniques used in carbohydrate analysis by CE. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements.

PubMed

Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per

2014-02-01

This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation. © 2013 Elsevier B.V. All rights reserved.

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.

Recent Advances in the Separation of Rare Earth Elements Using Mesoporous Hybrid Materials.

PubMed

Hu, Yimu; Florek, Justyna; Larivière, Dominic; Fontaine, Frédéric-Georges; Kleitz, Freddy

2018-05-27

Over the past decades, the need for rare earth elements (REEs) has increased substantially, mostly because these elements are used as valuable additives in advanced technologies. However, the difference in ionic radius between neighboring REEs is small, which renders an efficient sized-based separation extremely challenging. Among different types of extraction methods, solid-phase extraction (SPE) is a promising candidate, featuring high enrichment factor, rapid adsorption kinetics, reduced solvent consumption and minimized waste generation. The great challenge remains yet to develop highly efficient and selective adsorbents for this process. In this regard, ordered mesoporous materials (OMMs) possess high specific surface area, tunable pore size, large pore volume, as well as stable and interconnected frameworks with active pore surfaces for functionalization. Such features meet the requirements for enhanced adsorbents, not only providing huge reactional interface and large surface capable of accommodating guest species, but also enabling the possibility of ion-specific binding for enrichment and separation purposes. This short personal account summarizes some of the recent advances in the use of porous hybrid materials as selective sorbents for REE separation and purification, with particular attention devoted to ordered mesoporous silica and carbon-based sorbents. © 2018 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

METHOD OF SEPARATING HYDROGEN ISOTOPES

DOEpatents

Salmon, O.N.

1958-12-01

The process of separating a gaseous mixture of hydrogen and tritium by contacting finely dlvided palladium with the mixture in order to adsorb the gases, then gradually heating the palladium and collecting the evolved fractlons, is described. The fraction first given off is richer in trltium than later fractions.

Characterization of diesel fuel by chemical separation combined with capillary gas chromatography (GC) isotope ratio mass spectrometry (IRMS).

PubMed

Harvey, Scott D; Jarman, Kristin H; Moran, James J; Sorensen, Christina M; Wright, Bob W

2012-09-15

The purpose of this study was to perform a preliminary investigation of compound-specific isotope analysis (CSIA) of diesel fuels to evaluate whether the technique could distinguish diesel samples from different sources/locations. The ability to differentiate or correlate diesel samples could be valuable for discovering fuel tax evasion schemes or for environmental forensic studies. Two urea adduction-based techniques were used to isolate the n-alkanes from the fuel. Both carbon isotope ratio (δ(13)C) and hydrogen isotope ratio (δD) values for the n-alkanes were then determined by CSIA in each sample. The samples investigated had δ(13)C values that ranged from -30.1‰ to -26.8‰, whereas δD values ranged from -83‰ to -156‰. Plots of δD versus δ(13)C with sample n-alkane points connected in order of increasing carbon number gave well-separated clusters with characteristic shapes for each sample. Principal components analysis (PCA) with δ(13)C, δD, or combined δ(13)C and δD data was applied to extract the maximum information content. PCA scores plots could clearly differentiate the samples, thereby demonstrating the potential of this approach for distinguishing (e.g., fingerprinting) fuel samples using δ(13)C and δD values. Copyright © 2012 Elsevier B.V. All rights reserved.

Investigation of Isotopically Tailored Boron in Advanced Fission and Fusion Reactor Systems.

NASA Astrophysics Data System (ADS)

Domaszek, Gerald Raymond

effectiveness of various materials as reflector control elements for a compact space reactor has shown that B^{11} is neutronically superior to graphite in these applications. Metallic boron and boron carbide isotopically enriched in B^{11} have been demonstrated to be neutronically acceptable for varied applications in advanced reactor systems. B^ {11} has been shown to be superior in performance to graphite. While only somewhat inferior to beryllium as neutron multipliers, B^ {11} and B^{11} _4C have safety, supply and cost advantage over beryllium. (Abstract shortened with permission of author.).

[Baseflow separation methods in hydrological process research: a review].

PubMed

Xu, Lei-Lei; Liu, Jing-Lin; Jin, Chang-Jie; Wang, An-Zhi; Guan, De-Xin; Wu, Jia-Bing; Yuan, Feng-Hui

2011-11-01

Baseflow separation research is regarded as one of the most important and difficult issues in hydrology and ecohydrology, but lacked of unified standards in the concepts and methods. This paper introduced the theories of baseflow separation based on the definitions of baseflow components, and analyzed the development course of different baseflow separation methods. Among the methods developed, graph separation method is simple and applicable but arbitrary, balance method accords with hydrological mechanism but is difficult in application, whereas time series separation method and isotopic method can overcome the subjective and arbitrary defects caused by graph separation method, and thus can obtain the baseflow procedure quickly and efficiently. In recent years, hydrological modeling, digital filtering, and isotopic method are the main methods used for baseflow separation.

System for recovery of daughter isotopes from a source material

DOEpatents

Tranter, Troy J [Idaho Falls, ID; Todd, Terry A [Aberdeen, ID; Lewis, Leroy C [Idaho Falls, ID; Henscheid, Joseph P [Idaho Falls, ID

2009-08-04

A method of separating isotopes from a mixture containing at least two isotopes in a solution is disclosed. A first isotope is precipitated and is collected from the solution. A daughter isotope is generated and collected from the first isotope. The invention includes a method of producing an actinium-225/bismuth-213 product from a material containing thorium-229 and thorium-232. A solution is formed containing nitric acid and the material containing thorium-229 and thorium-232, and iodate is added to form a thorium iodate precipitate. A supernatant is separated from the thorium iodate precipitate and a second volume of nitric acid is added to the thorium iodate precipitate. The thorium iodate precipitate is stored and a decay product comprising actinium-225 and bismuth-213 is generated in the second volume of nitric acid, which is then separated from the thorium iodate precipitate, filtered, and treated using at least one chromatographic procedure. A system for producing an actinium-225/bismuth-213 product is also disclosed.

Rare Isotopes Physics in the Multimessenger Era

NASA Astrophysics Data System (ADS)

Schatz, Hendrik

2018-06-01

While these isotopes only exist for fractions of seconds, their properties shape the resulting cosmic distribution of elements and the astronomical observables including spectra, neutrinos, and gravitational waves. The long standing challenge in nuclear astrophysics of the production of the relevant isotopes in the laboratory is now overcome with a new generation of rare isotope accelerator facilities now coming online. One example is the FRIB facility under construction at Michigan State University for the US Department of Energy, Office of Science, Office of Nuclear Physics. These new capabilities in nuclear physics coincide with advances in astronomy directly related to the cosmic sites where these isotopes are created, in particular in time domain and gravitational wave astronomy. I will discuss the importance of rare isotope physics in interpreting multi-messenger observations and how advances in nuclear physics and astronomy when combined promise to lead us towards a comprehensive theory of the origin of the elements.

The beam diagnostic instruments in Beijing radioactive ion-beam facilities isotope separator on-line

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ma, Y., E-mail: yjma@ciae.ac.cn; Cui, B.; Ma, R.

The beam diagnostic instruments for Beijing Radioactive Ion-beam Facilities Isotope Separator On-Line are introduced [B. Q. Cui, Z. H. Peng, Y. J. Ma, R. G. Ma, B. Tang, T. Zhang, and W. S. Jiang, Nucl. Instrum. Methods 266, 4113 (2008); T. J. Zhang, X. L. Guan, and B. Q. Cui, in Proceedings of APAC 2004, Gyeongju, Korea, 2004, http://www.jacow.org , p. 267]. For low intensity ion beam [30–300 keV/1 pA–10 μA], the beam profile monitor, the emittance measurement unit, and the analyzing slit will be installed. For the primary proton beam [100 MeV/200 μA], the beam profile scanner will bemore » installed. For identification of the nuclide, a beam identification unit will be installed. The details of prototype of the beam diagnostic units and some experiment results will be described in this article.« less

Golan Heights Groundwater Systems: Separation By REE+Y And Stable Isotopes

NASA Astrophysics Data System (ADS)

Siebert, C.; Geyer, S.; Knoeller, K.; Roediger, T.; Weise, S.; Dulski, P.; Moeller, P.; Guttman, J.

2008-12-01

In a semi-arid to arid country like Israel, all freshwater resources are under (over-) utilization. Particularly, the Golan Heights rank as one of the most important extraction areas of groundwater of good quality and quantity. Additionally the mountain range feed to a high degree the most important freshwater reservoir of Israel, the Sea of Galilee. Hence, knowing the sources and characters of the Golan Heights groundwater systems is an instantaneous demand regarding sustainable management and protection. Within the "German-Israeli-Jordanian-Palestinian Joint Research Program for the Sustainable Utilisation of Aquifer Systems", hundreds of water samples were taken from all over the Jordan-Dead Sea rift-system to understand groundwater flow-systems and salinisation. For that purpose, each sample was analysed for major and minor ions, rare earth elements including yttrium (REY) and stable isotopes of water (d18O, d2H). The REY distribution in groundwater is established during infiltration by the first water-rock interaction and consequently reflects the leachable components of sediments and rocks of the recharge area. In well- developed flow-systems, REY are adsorbed onto pore surfaces are in equilibrium with the percolating groundwater, even if the lithology changes (e.g. inter-aquifer flow). Thus, groundwater sampled from wells and springs still show the REY distribution pattern established in the recharge area. Since high temperatures do not occur in Golan Heights, d2H and d18O are less controlled by water-rock interaction than by climatic and geomorphological factors at the time of replenishment. Applying the REY signature as a grouping criterion of groundwaters, d18O vs. d2H plots yield a new dimension in interpreting isotope data. The combined use of hydrochemical and isotopic methods enabled us to contain the areas of replenishment and the flow-paths of all investigated groundwater in the Golan Heights. Despite location, salinity or temperature of spring or

High-Precision Measurement of 13C/12C Isotopic Ratio Using Gas Chromatography-Combustion-Cavity Ring-Down Spectroscopy

NASA Astrophysics Data System (ADS)

Saad, N.; Kuramoto, D. S.; Haase, C.; Crosson, E.; Tan, S.; Zare, R. N.

2009-12-01

combusted products were combined with dry nitrogen gas to provide sufficient gas flow for the CRDS analyzer, which measured the 13C/12C isotopic ratio of the separated methane, ethane, and propane, obtaining a precision of 0.95 permil or better. The calibration accuracy was within 3 permil of the values determined using IRMS. The current CRDS-based system is less expensive, does not require highly trained personnel to operate, and is portable, compared with IRMS. We anticipate that advances in spectroscopic analysis will improve the precision and accuracy of the CRDS isotopic measurement, making it comparable with IRMS.

Compound-specific nitrogen isotope analysis of D-alanine, L-alanine, and valine: application of diastereomer separation to delta15N and microbial peptidoglycan studies.

PubMed

Takano, Yoshinori; Chikaraishi, Yoshito; Ogawa, Nanako O; Kitazato, Hiroshi; Ohkouchi, Naohiko

2009-01-01

We have developed an analytical method to determine the compound-specific nitrogen isotope compositions of individual amino acid enantiomers using gas chromatography/combustion/isotope ratio mass spectrometry. A novel derivatization of amino acid diastereomers by optically active (R)-(-)-2-butanol or (S)-(+)-2-butanol offers two advantages for nitrogen isotope analysis. First, chromatographic chiral separation can be achieved without the use of chiral stationary-phase columns. Second, the elution order of these compounds on the chromatogram can be switched by a designated esterification reaction. We applied the method to the compound-specific nitrogen isotope analysis of D- and L-alanine in a peptidoglycan derived from the cell walls of cultured bacteria (Firmicutes and Actinobacteria; Enterococcus faecalis, Staphylococcus aureus, Staphylococcus staphylolyticus, Lactobacillus acidophilus, Bacillus subtilis, Micrococcus luteus, and Streptomyces sp.), natural whole bacterial cells (Bacillus subtilis var. natto), (pseudo)-peptidoglycan from archaea (Methanobacterium sp.), and cell wall from eukaryota (Saccharomyces cerevisiae). We observed statistically significant differences in nitrogen isotopic compositions; e.g., delta15N ( per thousand vs air) in Staphylococcus staphylolyticus for d-alanine (19.2 +/- 0.5 per thousand, n = 4) and L-alanine (21.3 +/- 0.8 per thousand, n = 4) and in Bacillus subtilis for D-alanine (6.2 +/- 0.2 per thousand, n = 3) and L-alanine (8.2 +/- 0.4 per thousand, n = 3). These results suggest that enzymatic reaction pathways, including the alanine racemase reaction, produce a nitrogen isotopic difference in amino acid enantiomers, resulting in 15N-depleted D-alanine. This method is expected to facilitate compound-specific nitrogen isotope studies of amino acid stereoisomers.

Efficient 3He/4He separation in a nanoporous graphenylene membrane.

PubMed

Qu, Yuanyuan; Li, Feng; Zhao, Mingwen

2017-08-16

Helium-3 is a precious noble gas, which is essential in many advanced technologies such as cryogenics, isotope labeling and nuclear weapons. The current imbalance of 3 He demand and supply shortage leads to the search for an efficient membrane with high performance for 3 He separation. In this study, based on first-principles calculations, we demonstrated that highly efficient 3 He harvesting can be achieved in a nanoporous graphenylene membrane with industrially-acceptable selectivity and permeance. The quantum tunneling effect leads to 3 He harvesting with high efficiency via kinetic sieving. Both the quantum tunneling effect and zero-point energy (ZPE) determine the 3 He/ 4 He separation via thermally-driven equilibrium sieving, where the ZPE effect dominates efficient 3 He/ 4 He separation between two reservoirs. The quantum effects revealed in this work suggest that the nanoporous graphenylene membrane is promising for efficient 3 He harvesting that can be exploited for industrial applications.

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...

Advances in electrophoretic separations

NASA Technical Reports Server (NTRS)

Snyder, R. S.; Rhodes, P. H.

1984-01-01

Free fluid electrophoresis is described using laboratory and space experiments combined with extensive mathematical modeling. Buoyancy driven convective flows due to thermal and concentration gradients are absent in the reduced gravity environment of space. The elimination of convection in weightlessness offers possible improvements in electrophoresis and other separation methods which occur in fluid media. The mathematical modeling suggests new ways of doing electrophoresis in space and explains various phenomena observed during past experiments. The extent to which ground based separation techniques are limited by gravity induced convection is investigated and space experiments are designed to evaluate specific characteristics of the fluid/particle environment. A series of experiments are proposed that require weightlessness and apparatus is developed that can be used to carry out these experiments in the near future.

Recent advances in monolithic columns for protein and peptide separation by capillary liquid chromatography.

PubMed

Liang, Yu; Zhang, Lihua; Zhang, Yukui

2013-03-01

Capillary liquid chromatography (cLC) has great potential for protein and peptide separation, with advantages of high efficiency, high resolution, low sample consumption, and high sensitivity when coupled with mass spectrometry. In recent years, monoliths have been widely used as the stationary phases for capillary columns, owing to easy preparation, high permeability, fast mass transfer, and low backpressure. This review summarizes recent advances (2007-2012) in monolithic columns for protein and peptide separation by cLC. After a brief introduction on the preparation of monolithic capillary columns, the emphasis of this review is focused on the recent application of such columns for protein and peptide separation by cLC. Furthermore, the challenges and potential hot points of monolithic capillary columns in the future are discussed.

Calculations on Isotope Separation by Laser Induced Photodissociation of Polyatomic Molecules. Final Report

DOE R&D Accomplishments Database

Lamb, W. E. Jr.

1978-11-01

This report describes research on the theory of isotope separation produced by the illumination of polyatomic molecules by intense infrared laser radiation. Newton`s equations of motion were integrated for the atoms of the SF{sub 6} molecule including the laser field interaction. The first year`s work has been largely dedicated to obtaining a suitable interatomic potential valid for arbitrary configurations of the seven particles. This potential gives the correct symmetry of the molecule, the equilibrium configuration, the frequencies of the six distinct normal modes of oscillation and the correct (or assumed) value of the total potential energy of the molecule. Other conditions can easily be imposed in order to obtain a more refined potential energy function, for example, by making allowance for anharmonicity data. A suitable expression was also obtained for the interaction energy between a laser field and the polyatomic molecule. The electromagnetic field is treated classically, and it would be easily possible to treat the cases of time dependent pulses, frequency modulation and noise.

Photonuclear Production of Medical Isotopes

NASA Astrophysics Data System (ADS)

Weinandt, Nick

2011-10-01

Every year, more than 20 million people in the United States receive a nuclear medicine procedure. Many of the isotopes needed for these procedures are under-produced. Suppliers of the isotopes are usually located outside the United States, which presents a problem when the desired isotopes have short half-lives. Linear accelerators were investigated as a possible method of meeting isotope demand. Linear accelerators are cheaper, safer, and have lower decommissioning costs compared to nuclear reactors. By using (γ,p) reactions, the desired isotope can be separated from the target material due to the different chemical nature of each isotope. Isotopes investigated were Cu-67, In-111, and Lu-111. Using the results the photon flux Monte Carlo simulations, the expected activity of isotopes can be calculated. After samples were irradiated, a high purity germanium detector and signal processing apparatus were used to count the samples. The activity at the time of irradiation stop was then calculated. The uses of medical isotopes will also be presented. Thanks to Idaho State University, the Idaho Accelerator Center, and the National Science Foundation for supporting the research.

New Fragment Separation Technology for Superheavy Element Research

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shaughnessy, D A; Moody, K J; Henderson, R A

2008-01-28

This project consisted of three major research areas: (1) development of a solid Pu ceramic target for the MASHA separator, (2) chemical separation of nuclear decay products, and (3) production of new isotopes and elements through nuclear reactions. There have been 16 publications as a result of this project, and this collection of papers summarizes our accomplishments in each of the three areas of research listed above. The MASHA (Mass Analyzer for Super-Heavy Atoms) separator is being constructed at the U400 Cyclotron at the Flerov Laboratory of Nuclear Reactions in Dubna, Russia. The purpose of the separator is to physicallymore » separate the products from nuclear reactions based on their isotopic masses rather than their decay characteristics. The separator was designed to have a separation between isotopic masses of {+-}0.25 amu, which would enable the mass of element 114 isotopes to be measured with outstanding resolution, thereby confirming their discovery. In order to increase the production rate of element 114 nuclides produced via the {sup 244}Pu+{sup 48}Ca reaction, a new target technology was required. Instead of a traditional thin actinide target, the MASHA separator required a thick, ceramic-based Pu target that was thick enough to increase element 114 production while still being porous enough to allow reaction products to migrate out of the target and travel through the separator to the detector array located at the back end. In collaboration with UNLV, we began work on development of the Pu target for MASHA. Using waste-form synthesis technology, we began by creating zirconia-based matrices that would form a ceramic with plutonium oxide. We used samarium oxide as a surrogate for Pu and created ceramics that had varying amounts of the starting materials in order to establish trends in material density and porosity. The results from this work are described in more detail in Refs. [1,4,10]. Unfortunately, work on MASHA was delayed in Russia because

Advances in laser ablation MC-ICPMS isotopic analysis of rock materials

NASA Astrophysics Data System (ADS)

Young, E. D.

2007-12-01

Laser ablation multiple-collector inductively coupled plasma-source mass spectrometry (LA-MC-ICPMS) is a rapid method for obtaining high-precision isotope ratio measurements in geological samples. The method has been used with success for measuring isotope ratios of numerous elements, including Pb, Hf, Mg, Si, and Fe in terrestrial and extraterrestrial samples. It fills the gap between the highest precision obtainable with acid digestion together with MC-ICPMS and thermal ionization mass spectrometry (TIMS) and the maximum spatial resolution afforded by secondary ion mass spectrometry (SIMS). Matrix effects have been shown to be negligible for Pb isotopic analysis by LA-MC-ICPMS (Simon et al., 2007). Glass standards NBS 610, 612, and 614 have Pb/matrix ratios spanning two orders of magnitude. Our sample-standard bracketing laser ablation technique gives accurate and precise 208Pb/206Pb and 207Pb/206Pb for these glasses. The accuracy is superior to that obtained when using Tl to correct for mass fractionation. Accuracy and precision (± 0.2 ‰) for Pb in feldspars is comparable to that for double-spike TIMS. Data like these have been used to distinguish distinct sources of magmas in the Long Valley silicic magma system. LA-MC-ICPMS analyses of Mg isotope ratios in calcium-aluminum-rich inclusions (CAIs) from carbonaceous chondrite meteorites have revealed a wealth of new information about the history of these objects. A byproduct of this work has been recognition of the importance of different mass fractionation laws among three isotopes of a given element. Kinetic and equilibrium processes define distinct fractionation laws. Reservoir effects can further modify these laws. The result is that the linear coefficient β that relates the logarithms of the ratios n2/n1 and n3/n1 (ni refers to the number of atoms of isotope i) of isotopes with masses m3 > m2 > m1 is not unique. Rather, it is process dependent. In the case of Mg, this coefficient ranges from 0.521 for

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.

Advances in Multicollector ICPMS for precise and accurate isotope ratio measurements of Uranium isotopes

NASA Astrophysics Data System (ADS)

Bouman, C.; Lloyd, N. S.; Schwieters, J.

2011-12-01

The accurate and precise determination of uranium isotopes is challenging, because of the large dynamic range posed by the U isotope abundances and the limited available sample material. Various mass spectrometric techniques are used for the measurement of U isotopes, where TIMS is the most accepted and accurate one. Multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) can offer higher productivity compared to TIMS, but is traditionally limited by low efficiency of sample utilisation. This contribution will discuss progress in MC-ICPMS for detecting 234U, 235U, 236U and 238U in various uranium reference materials from IRMM and NBL. The Thermo Scientific NEPTUNE Plus with Jet Interface offers a modified dry plasma ICP interface using a large interface pump combined with a special set of sample and skimmer cones giving ultimate sensitivity for all elements across the mass range. For uranium, an ion yield of > 3 % was reported previously [1]. The NEPTUNE Plus also offers Multi Ion Counting using discrete dynode electron multipliers as well as two high abundance-sensitivity filters to discriminate against peak tailing effects on 234U and 236U originating from the major uranium beams. These improvements in sensitivity and dynamic range allow accurate measurements of 234U, 235U and 236U abundances on very small samples and at low concentration. In our approach, minor U isotopes 234U and 236U were detected on ion counters with high abundance sensitivity filters, whereas 235U and 238U were detected on Faraday Cups using a high gain current amplifier (10e12 Ohm) for 235U. Precisions and accuracies for 234U and 236U were down to ~1%. For 235U, subpermil levels were reached.

Carbon isotope ratios and isotopic correlations between components in fruit juices

NASA Astrophysics Data System (ADS)

Wierzchnicki, Ryszard

2013-04-01

Nowadays food products are defined by geographical origin, method of production and by some regulations concerning terms of their authenticity. Important data for confirm the authenticity of product are providing by isotopic methods of food control. The method checks crucial criteria which characterize the authenticity of inspected product. The European Union Regulations clearly show the tendency for application of the isotopic methods for food authenticity control (wine, honey, juice). The aim of the legislation steps is the protection of European market from possibility of the commercial frauds. Method of isotope ratio mass spectrometry is very effective tool for the use distinguishably the food products of various geographical origin. The basic problem for identification of the sample origin is the lack of databases of isotopic composition of components and information about the correlations of the data. The subject of the work was study the isotopic correlations existing between components of fruits. The chemical and instrumental methods of separation: water, sugars, organic acids and pulp from fruit were implemented. IRMS technique was used to measure isotopic composition of samples. The final results for original samples of fruits (apple, strawberry etc.) will be presented and discussed. Acknowledgement: This work was supported by the Polish Ministry of Science and Higher Education under grant NR12-0043-10/2010.

An in-advance stable isotope labeling strategy for relative analysis of multiple acidic plant hormones in sub-milligram Arabidopsis thaliana seedling and a single seed.

PubMed

Sun, Xiaohong; Ouyang, Yue; Chu, Jinfang; Yan, Jing; Yu, Yan; Li, Xiaoqiang; Yang, Jun; Yan, Cunyu

2014-04-18

A sensitive and reliable in-advance stable isotope labeling strategy was developed for simultaneous relative quantification of 8 acidic plant hormones in sub-milligram amount of plant materials. Bromocholine bromide (BETA) and its deuterated counterpart D9-BETA were used to in-advance derivatize control and sample extracts individually, which were then combined and subjected to solid-phase extraction (SPE) purification followed by UPLC-MS/MS analysis. Relative quantification of target compounds was obtained by calculation of the peak area ratios of BETA/D9-BETA labeled plant hormones. The in-advance stable isotope labeling strategy realized internal standard-based relative quantification of multiple kinds of plant hormones independent of availability of internal standard of every analyte with enhanced sensitivity of 1-3 orders of magnitude. Meanwhile, the in-advance labeling contributes to higher sample throughput and more reliability. The method was successfully applied to determine 8 plant hormones in 0.8mg DW (dry weight) of seedlings and 4 plant hormones from single seed of Arabidopsis thaliana. The results show the potential of the method in relative quantification of multiple plant hormones in tiny plant tissues or organs, which will advance the knowledge of the crosstalk mechanism of plant hormones. Copyright © 2014 Elsevier B.V. All rights reserved.

Mantle Helium and Carbon Isotopes in Separation Creek Geothermal Springs, Three Sisters Area, Central Oregon: Evidence for Renewed Volcanic Activity or a Long Term Steady State System?

USGS Publications Warehouse

Van Soest, M. C.; Kennedy, B.M.; Evans, William C.; Mariner, R.H.

2002-01-01

Here we present the helium and carbon isotope results from the initial study of a fluid chemistry-monitoring program started in the summer of 2001 near the South Sister volcano in central Oregon. The Separation Creek area which is several miles due west of the volcano is the locus of strong crustal uplift currently occurring at a rate of 4-5 cm/yr (Wicks, et. al., 2001).Helium [RC/RA = 7.44 and 8.61 RA (RC/R A = (3He/4He)sample-. air corrected/(3He/4He)air))] and carbon (??13C = -11.59 to -9.03??? vs PDB) isotope data and CO2/3He (5 and 9 ?? 109) show that bubbling cold springs in the Separation Creek area near South Sister volcano carry a strong mantle signal, indicating the presence of fresh basaltic magma in the volcanic plumbing system. There is no evidence though, to directly relate this signal to the crustal uplift that is currently taking place in the area, which started in 1998. The geothermal system in the area is apparently much longer lived and shows no significant changes in chemistry compared to data from the early 1990s. Hot springs in the area, which are relatively far removed from the volcanic edifice, do not carry a strong mantle signal in helium isotope ratios (2.79 to 5.08 RA), unlike the cold springs, and also do not show any significant changes in helium isotope ratios compared to literature data for the same springs of over two decades ago. The cold springs of the Separation Creek area form a very diffuse but significant low temperature geothermal system, that should, due to its close vicinity to the center of up uplift, be more sensitive to changes in the deeper volcanic plumbing system than the far removed hot springs and therefore require much more study and consideration when dealing with volcano monitoring in the Cascade range or possibly with geothermal exploration in general.

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.

Improvement of Pt/C/PTFE catalyst type used for hydrogen isotope separation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vasut, F.; Preda, A.; Zamfirache, M.

2008-07-15

The CANDU reactor from the Nuclear Power plant Cernavoda (Romania)) is the most powerful tritium source from Europe. This reactor is moderated and cooled by heavy water that becomes continuously contaminated with tritium. Because of this reason, the National R and amp;D Inst. for Cryogenic and Isotopic Technologies developed a detritiation technology based on catalytic isotopic exchange and cryogenic distillation. The main effort of our Inst. was focused on finding more efficient catalysts with a longer operational life. Some of the tritium removal processes involved in Fusion Science and Technology use this type of catalyst 1. Several Pt/C/PTFE hydrophobic catalystsmore » that could be used in isotopic exchange process 2,3,4 were produced. The present paper presents a comparative study between the physical and morphological properties of different catalysts manufactured by impregnation at our institute. The comparison consists of a survey of specific surface, pores volume and pores distribution. (authors)« less

[Determination of 235U/238U isotope ratios in camphor tree bark samples by MC-ICP-MS after separation of uranium from matrix elements].

PubMed

Wang, Xiao-Ping; Zhang, Ji-Long

2007-07-01

Twelve camphor (cinnamomum camphora) tree bark samples were collected from Hiroshima and Kyoto, and the matrix element composition and morphology of the outer surface of these camphor tree bark samples were studied by EDXS and SEM respectively. After a dry decomposition, DOWEX 1-X8 anion exchange resin was used to separate uranium from matrix elements in these camphor tree bark samples. Finally, 235U/238 U isotope ratios in purified uranium solutions were determined by MC-ICP-MS. It was demonstrated that the outer surface of these camphor tree bark samples is porous and rough, with Al, Ca, Fe, K, Mg, Si, C, O and S as its matrix element composition. Uranium in these camphor tree bark samples can be efficiently separated and quantitatively recovered from the matrix element composition. Compared with those collected from Kyoto, the camphor tree bark samples collected from Hiroshima have significantly higher uranium contents, which may be due to the increased aerosol mass concentration during the city reconstruction. Moreover, the 235 U/23.U isotope ratios in a few camphor tree bark samples collected from Hiroshima are slightly higher than 0.007 25.

Using isotopes of dissolved inorganic carbon species and water to separate sources of recharge in a cave spring, northwestern Arkansas, USA Blowing Spring Cave

USGS Publications Warehouse

Knierim, Katherine J.; Pollock, Erik; Hays, Phillip D.

2013-01-01

Blowing Spring Cave in northwestern Arkansas is representative of cave systems in the karst of the Ozark Plateaus, and stable isotopes of water (δ18O and δ2H) and inorganic carbon (δ13C) were used to quantify soil-water, bedrock-matrix water, and precipitation contributions to cave-spring flow during storm events to understand controls on cave water quality. Water samples from recharge-zone soils and the cave were collected from March to May 2012 to implement a multicomponent hydrograph separation approach using δ18O and δ2H of water and dissolved inorganic carbon (δ13C–DIC). During baseflow, median δ2H and δ18O compositions were –41.6‰ and –6.2‰ for soil water and were –37.2‰ and –5.9‰ for cave water, respectively. Median DIC concentrations for soil and cave waters were 1.8 mg/L and 25.0 mg/L, respectively, and median δ13C–DIC compositions were –19.9‰ and –14.3‰, respectively. During a March storm event, 12.2 cm of precipitation fell over 82 h and discharge increased from 0.01 to 0.59 m3/s. The isotopic composition of precipitation varied throughout the storm event because of rainout, a change of 50‰ and 10‰ for δ2H and δ18O was observed, respectively. Although, at the spring, δ2H and δ18O only changed by approximately 3‰ and 1‰, respectively. The isotopic compositions of precipitation and pre-event (i.e., soil and bedrock matrix) water were isotopically similar and the two-component hydrograph separation was inaccurate, either overestimating (>100%) or underestimating (<0%) the precipitation contribution to the spring. During the storm event, spring DIC and δ13C–DIC decreased to a minimum of 8.6 mg/L and –16.2‰, respectively. If the contribution from precipitation was assumed to be zero, soil water was found to contribute between 23 to 72% of the total volume of discharge. Although the assumption of negligible contributions from precipitation is unrealistic, especially in karst systems where rapid flow

Method and apparatus for tritiated water separation

DOEpatents

Nelson, David A.; Duncan, James B.; Jensen, George A.

1995-01-01

The present invention is a membrane method and apparatus for separating isotopic water constituents from light water. The method involves providing a supported membrane of an aromatic polyphosphazene and pressurizing the water on one side of the membrane thereby forcing the light water through the supported membrane while isotopic water constituents are retained or vice versa. The apparatus of the present invention includes an aromatic polyphosphazene placed on a porous support and means for pressurizing water through the membrane while certain isotopic water constituents are retained.

Future Opportunities at the Facility for Rare Isotope Beams

NASA Astrophysics Data System (ADS)

Sherrill, Bradley M.

2018-05-01

This paper overviews the Facility for Rare Isotope Beams, FRIB, its construction status at the time of the conference, and its scientific program. FRIB is based on a high-power, heavy-ion, superconducting linear accelerator that is designed to deliver at least 400kW at 200 MeV/u for all stable-ion beams and produce a large fraction of all possible isotopes of the elements. A three-stage fragment separator will separate rare isotope beams for use in experiments at high energy or stopped and reaccelerated to up to 10MeV/u. The facility is expected to have first beams in 2021. An overview of the planned scientific program, experimental capabilities, and equipment initiatives are presented.

Process for producing enriched uranium having a .sup.235 U content of at least 4 wt. % via combination of a gaseous diffusion process and an atomic vapor laser isotope separation process to eliminate uranium hexafluoride tails storage

DOEpatents

Horton, James A.; Hayden, Jr., Howard W.

1995-01-01

An uranium enrichment process capable of producing an enriched uranium, having a .sup.235 U content greater than about 4 wt. %, is disclosed which will consume less energy and produce metallic uranium tails having a lower .sup.235 U content than the tails normally produced in a gaseous diffusion separation process and, therefore, eliminate UF.sub.6 tails storage and sharply reduce fluorine use. The uranium enrichment process comprises feeding metallic uranium into an atomic vapor laser isotope separation process to produce an enriched metallic uranium isotopic mixture having a .sup.235 U content of at least about 2 wt. % and a metallic uranium residue containing from about 0.1 wt. % to about 0.2 wt. % .sup.235 U; fluorinating this enriched metallic uranium isotopic mixture to form UF.sub.6 ; processing the resultant isotopic mixture of UF.sub.6 in a gaseous diffusion process to produce a final enriched uranium product having a .sup.235 U content of at least 4 wt. %, and up to 93.5 wt. % or higher, of the total uranium content of the product, and a low .sup.235 U content UF.sub.6 having a .sup.235 U content of about 0.71 wt. % of the total uranium content of the low .sup.235 U content UF.sub.6 ; and converting this low .sup.235 U content UF.sub.6 to metallic uranium for recycle to the atomic vapor laser isotope separation process.

Process for producing enriched uranium having a {sup 235}U content of at least 4 wt. % via combination of a gaseous diffusion process and an atomic vapor laser isotope separation process to eliminate uranium hexafluoride tails storage

DOEpatents

Horton, J.A.; Hayden, H.W. Jr.

1995-05-30

An uranium enrichment process capable of producing an enriched uranium, having a {sup 235}U content greater than about 4 wt. %, is disclosed which will consume less energy and produce metallic uranium tails having a lower {sup 235}U content than the tails normally produced in a gaseous diffusion separation process and, therefore, eliminate UF{sub 6} tails storage and sharply reduce fluorine use. The uranium enrichment process comprises feeding metallic uranium into an atomic vapor laser isotope separation process to produce an enriched metallic uranium isotopic mixture having a {sup 235} U content of at least about 2 wt. % and a metallic uranium residue containing from about 0.1 wt. % to about 0.2 wt. % {sup 235} U; fluorinating this enriched metallic uranium isotopic mixture to form UF{sub 6}; processing the resultant isotopic mixture of UF{sub 6} in a gaseous diffusion process to produce a final enriched uranium product having a {sup 235}U content of at least 4 wt. %, and up to 93.5 wt. % or higher, of the total uranium content of the product, and a low {sup 235}U content UF{sub 6} having a {sup 235}U content of about 0.71 wt. % of the total uranium content of the low {sup 235}U content UF{sub 6}; and converting this low {sup 235}U content UF{sub 6} to metallic uranium for recycle to the atomic vapor laser isotope separation process. 4 figs.

First calibration measurements of an FTIR absorption spectroscopy system for liquid hydrogen isotopologues for the isotope separation system of fusion power plants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Groessle, R.; Beck, A.; Bornschein, B.

2015-03-15

Fusion facilities like ITER and DEMO will circulate huge amounts of deuterium and tritium in their fuel cycle with an estimated throughput of kg per hour. One important capability of these fuel cycles is to separate the hydrogen isotopologues (H{sub 2}, D{sub 2}, T{sub 2}, HD, HT, DT). For this purpose the Isotope Separation System (ISS), using cryogenic distillation, as part of the Tritium Enrichment Test Assembly (TRENTA) is under development at Tritium Laboratory Karlsruhe. Fourier transform infrared absorption spectroscopy (FTIR) has been selected to prove its capability for online monitoring of the tritium concentration in the liquid phase atmore » the bottom of the distillation column of the ISS. The actual research-development work is focusing on the calibration of such a system. Two major issues are the identification of appropriate absorption lines and their dependence on the isotopic concentrations and composition. For this purpose the Tritium Absorption IR spectroscopy experiment has been set up as an extension of TRENTA. For calibration a Raman spectroscopy system is used. First measurements, with equilibrated mixtures of H{sub 2}, D{sub 2} and HD demonstrate that FTIR can be used for quantitative analysis of liquid hydro-gen isotopologues and reveal a nonlinear dependence of the integrated absorbance from the D{sub 2} concentration in the second vibrational branch of D{sub 2} FTIR spectra. (authors)« less

Method and apparatus for tritiated water separation

DOEpatents

Nelson, D.A.; Duncan, J.B.; Jensen, G.A.

1995-09-19

The present invention is a membrane method and apparatus for separating isotopic water constituents from light water. The method involves providing a supported membrane of an aromatic polyphosphazene and pressurizing the water on one side of the membrane thereby forcing the light water through the supported membrane while isotopic water constituents are retained or vice versa. The apparatus of the present invention includes an aromatic polyphosphazene placed on a porous support and means for pressurizing water through the membrane while certain isotopic water constituents are retained. 1 fig.

Accuracy of delta 18O isotope ratio measurements on the same sample by continuous-flow isotope-ratio mass spectrometry

USDA-ARS?s Scientific Manuscript database

The doubly labeled water method is considered the reference method to measure energy expenditure. Conventional mass spectrometry requires a separate aliquot of the same sample to be prepared and analyzed separately. With continuous-flow isotope-ratio mass spectrometry, the same sample could be analy...

Hafnium isotope stratigraphy of ferromanganese crusts

PubMed

Lee; Halliday; Hein; Burton; Christensen; Gunther

1999-08-13

A Cenozoic record of hafnium isotopic compositions of central Pacific deep water has been obtained from two ferromanganese crusts. The crusts are separated by more than 3000 kilometers but display similar secular variations. Significant fluctuations in hafnium isotopic composition occurred in the Eocene and Oligocene, possibly related to direct advection from the Indian and Atlantic oceans. Hafnium isotopic compositions have remained approximately uniform for the past 20 million years, probably reflecting increased isolation of the central Pacific. The mechanisms responsible for the increase in (87)Sr/(86)Sr in seawater through the Cenozoic apparently had no effect on central Pacific deep-water hafnium.

Membrane contactor/separator for an advanced ozone membrane reactor for treatment of recalcitrant organic pollutants in water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chan, Wai Kit, E-mail: kekyeung@ust.hk; Joueet, Justine; Heng, Samuel

An advanced ozone membrane reactor that synergistically combines membrane distributor for ozone gas, membrane contactor for pollutant adsorption and reaction, and membrane separator for clean water production is described. The membrane reactor represents an order of magnitude improvement over traditional semibatch reactor design and is capable of complete conversion of recalcitrant endocrine disrupting compounds (EDCs) in water at less than three minutes residence time. Coating the membrane contactor with alumina and hydrotalcite (Mg/Al=3) adsorbs and traps the organics in the reaction zone resulting in 30% increase of total organic carbon (TOC) removal. Large surface area coating that diffuses surface chargesmore » from adsorbed polar organic molecules is preferred as it reduces membrane polarization that is detrimental to separation. - Graphical abstract: Advanced ozone membrane reactor synergistically combines membrane distributor for ozone, membrane contactor for sorption and reaction and membrane separator for clean water production to achieve an order of magnitude enhancement in treatment performance compared to traditional ozone reactor. Highlights: Black-Right-Pointing-Pointer Novel reactor using membranes for ozone distributor, reaction contactor and water separator. Black-Right-Pointing-Pointer Designed to achieve an order of magnitude enhancement over traditional reactor. Black-Right-Pointing-Pointer Al{sub 2}O{sub 3} and hydrotalcite coatings capture and trap pollutants giving additional 30% TOC removal. Black-Right-Pointing-Pointer High surface area coating prevents polarization and improves membrane separation and life.« less

Why we need a centralized repository for isotopic data

USDA-ARS?s Scientific Manuscript database

Stable isotopes encode the origin and integrate the history of matter; thus, their analysis offers tremendous potential to address questions across diverse scientific disciplines. Indeed, the broad applicability of stable isotopes, coupled with advancements in high-throughput analysis, have created ...

Variation in nitrate isotopic signatures in sewage for source apportionment with urbanization: a case study in Beijing, China.

PubMed

Xian, Chaofan; Ouyang, Zhiyun; Li, Yanmin; Xiao, Yang; Ren, Yufen

2016-11-01

Nitrate (NO 3 - ) pollution is a severe problem in urban aquatic systems especially within megacity undergoing rapid urbanization, and mostly, sewage is supposed as the prevailing NO 3 - source. A dual isotope approach (δ 15 N-NO 3 - and δ 18 O-NO 3 - ) was applied to explore the variation in NO 3 - isotopic signatures in sewage processed by wastewater treatment plants (WWTPs) in Beijing from 2014 to 2015. We found that the raw and treated sewage owned the different NO 3 - isotopic signatures, including δ 15 N from 1.1 to 24.7 ‰ and δ 18 O from 1.6 to 22.8 ‰ in raw sewage, as well as δ 15 N from 6.1 to 22.8 ‰ and δ 18 O from 1.6 to 13.2 ‰ in treated effluents. The WWTP processing would result in the enrichment of NO 3 - isotopic compositions in discharged effluents with NO 3 - concentrations increasing. Besides, advanced sewage treatment technology with more pollutant N reduction may raise the heavier NO 3 - isotopic compositions further. The NO 3 - isotope value ranges of urban sewage and manure should be separated, and the seasonal and tighter NO 3 - isotope value ranges are supposed to improve the accuracy of source apportionment. The NO 3 - isotope value ranges conducted in this study might provide useful information for tracing NO 3 - sources towards the implementation of efficient water pollution control in Beijing.

Advances in chiral separations by nonaqueous capillary electrophoresis in pharmaceutical and biomedical analysis.

PubMed

Ali, Imran; Sanagi, Mohd Marsin; Aboul-Enein, Hassan Y

2014-04-01

NACE is an alternative technique to aqueous CE in the chiral separations of partially soluble racemates. Besides, partially water-soluble or insoluble chiral selectors may be exploited in the enantiomeric resolution in NACE. The high reproducibility due to low Joule heat generation and no change in BGE concentration may make NACE a routine analytical technique. These facts attracted scientists to use NACE for the chiral resolution. The present review describes the advances in the chiral separations by NACE and its application in pharmaceutical and biomedical analysis. The emphasis has been given to discuss the selection of the chiral selectors and organic solvents, applications of NACE, comparison between NACE and aqueous CE, and chiral recognition mechanism. Besides, efforts have also been made to predict the future perspectives of NACE. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

METHOD OF SEPARATING ISOTOPES OF URANIUM IN A CALUTRON

DOEpatents

Jenkins, F.A.

1958-05-01

Mass separation devices of the calutron type and the use of uranium hexachloride as a charge material in the calutron ion source are described. The method for using this material in a mass separator includes heating the uranium hexachloride to a temperature in the range of 60 to 100 d C in a vacuum and thereby forming a vapor of the material. The vaporized uranium hexachloride is then ionized in a vapor ionizing device for subsequent mass separation processing.

Can the waiting-point nucleus 78Ni be studied at an on-line mass-separator?

NASA Astrophysics Data System (ADS)

Wöhr, A.; Andreyev, A.; Bijnens, N.; Breitenbach, J.; Franchoo, S.; Huyse, M.; Kudryavtsev, Y. A.; Piechaczek, A.; Raabe, R. R.; Reusen, I.; Vermeeren, L.; Van Duppen, P.

1997-02-01

Short-lived nickel isotopes have been studied using a chemically selective Ion Guide Laser Ion Source (IGLIS) based on resonance ionisation of atoms at the Leuven Isotope Separator On-Line (LISOL) separator. The decay properties of different Ni isotopes have been studied using β-γ-coincidences. Experimental production rates of proton induced fission of 238U are obtained for 69,71Ni. These numbers are in a strong disagreement with Silberg-Tsao calculations.

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.

U.S. Department of Energy Isotope Program

ScienceCinema

None

2018-01-16

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. PNNL’s Isotope Program operates in a multi-program category-2 nuclear facility, the Radiochemical Processing Laboratory (RPL), that contains 16 hot cells and 20 gloveboxes. As part of the DOE Isotope Program, the Pacific Northwest National Laboratory dispenses strontium-90, neptunium-237, radium-223, and thorium-227. PNNL’s Isotope Program uses a dedicated hot-cell for strontium-90 dispensing and a dedicated glovebox for radium-223 and thorium-227 dispensing. PNNL’s Isotope Program has access to state of the art analytical equipment in the RPL to support their research and production activities. DOE Isotope Program funded research at PNNL has advanced the application of automated radiochemistry for isotope such as zirconium-89 and astatine-211 in partnership with the University of Washington.

U.S. Department of Energy Isotope Program

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

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. PNNL’s Isotope Program operates in a multi-program category-2 nuclear facility, the Radiochemical Processing Laboratory (RPL), that contains 16 hot cells and 20 gloveboxes. As part of the DOE Isotope Program, the Pacific Northwestmore » National Laboratory dispenses strontium-90, neptunium-237, radium-223, and thorium-227. PNNL’s Isotope Program uses a dedicated hot-cell for strontium-90 dispensing and a dedicated glovebox for radium-223 and thorium-227 dispensing. PNNL’s Isotope Program has access to state of the art analytical equipment in the RPL to support their research and production activities. DOE Isotope Program funded research at PNNL has advanced the application of automated radiochemistry for isotope such as zirconium-89 and astatine-211 in partnership with the University of Washington.« less

Iron speciation and isotope fractionation during silicate weathering and soil formation in an alpine glacier forefield chronosequence

NASA Astrophysics Data System (ADS)

Kiczka, Mirjam; Wiederhold, Jan G.; Frommer, Jakob; Voegelin, Andreas; Kraemer, Stephan M.; Bourdon, Bernard; Kretzschmar, Ruben

2011-10-01

The chemical weathering of primary Fe-bearing minerals, such as biotite and chlorite, is a key step of soil formation and an important nutrient source for the establishment of plant and microbial life. The understanding of the relevant processes and the associated Fe isotope fractionation is therefore of major importance for the further development of stable Fe isotopes as a tracer of the biogeochemical Fe cycle in terrestrial environments. We investigated the Fe mineral transformations and associated Fe isotope fractionation in a soil chronosequence of the Swiss Alps covering 150 years of soil formation on granite. For this purpose, we combined for the first time stable Fe isotope analyses with synchrotron-based Fe-EXAFS spectroscopy, which allowed us to interpret changes in Fe isotopic composition of bulk soils, size fractions, and chemically separated Fe pools over time in terms of weathering processes. Bulk soils and rocks exhibited constant isotopic compositions along the chronosequence, whereas soil Fe pools in grain size fractions spanned a range of 0.4‰ in δ 56Fe. The clay fractions (<2 μm), in which newly formed Fe(III)-(hydr)oxides contributed up to 50% of the total Fe, were significantly enriched in light Fe isotopes, whereas the isotopic composition of silt and sand fractions, containing most of the soil Fe, remained in the range described by biotite/chlorite samples and bulk soils. Iron pools separated by a sequential extraction procedure covered a range of 0.8‰ in δ 56Fe. For all soils the lightest isotopic composition was observed in a 1 M NH 2OH-HCl-25% acetic acid extract, targeting poorly-crystalline Fe(III)-(hydr)oxides, compared with easily leachable Fe in primary phyllosilicates (0.5 M HCl extract) and Fe in residual silicates. The combination of the Fe isotope measurements with the speciation data obtained by Fe-EXAFS spectroscopy permitted to quantitatively relate the different isotope pools forming in the soils to the mineral

Flexible, High-Wettability and Fire-Resistant Separators Based on Hydroxyapatite Nanowires for Advanced Lithium-Ion Batteries.

PubMed

Li, Heng; Wu, Dabei; Wu, Jin; Dong, Li-Ying; Zhu, Ying-Jie; Hu, Xianluo

2017-11-01

Separators play a pivotal role in the electrochemical performance and safety of lithium-ion batteries (LIBs). The commercial microporous polyolefin-based separators often suffer from inferior electrolyte wettability, low thermal stability, and severe safety concerns. Herein, a novel kind of highly flexible and porous separator based on hydroxyapatite nanowires (HAP NWs) with excellent thermal stability, fire resistance, and superior electrolyte wettability is reported. A hierarchical cross-linked network structure forms between HAP NWs and cellulose fibers (CFs) via hybridization, which endows the separator with high flexibility and robust mechanical strength. The high thermal stability of HAP NW networks enables the separator to preserve its structural integrity at temperatures as high as 700 °C, and the fire-resistant property of HAP NWs ensures high safety of the battery. In particular, benefiting from its unique composition and highly porous structure, the as-prepared HAP/CF separator exhibits near zero contact angle with the liquid electrolyte and high electrolyte uptake of 253%, indicating superior electrolyte wettability compared with the commercial polyolefin separator. The as-prepared HAP/CF separator has unique advantages of superior electrolyte wettability, mechanical robustness, high thermal stability, and fire resistance, thus, is promising as a new kind of separator for advanced LIBs with enhanced performance and high safety. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantifying weathering advance rates in basaltic andesite rinds with uranium-series isotopes: a case study from Guadeloupe

NASA Astrophysics Data System (ADS)

Ma, L.; Chabaux, F. J.; Pelt, E.; Granet, M.; Sak, P. B.; Gaillardet, J.; Brantley, S. L.

2010-12-01

-series activity ratios in the clast were modeled with a weathering advance rate of ~0.3 mm kyr-1. This represents the rind advance rate at the low curvature segment of the core-rind boundary under tropical climate. This rate is consistent with the previously estimated formation rates of basaltic rinds under similar tropic conditions in Costa Rica [Sak et al., 2004, GCA 68, 1453; Pelt et al., 2008, EPSL 276, 98]. This rate is about one order of magnitude greater than those in temperate regions, documenting the important control of temperature on basalt weathering. This work illustrates that the weathering advance rates of rinds can be successfully estimated by U-series isotopes, demonstrating their great potential as dating tools for Earth surface processes. Furthermore, U-series chronometry provides a suitable method for independently testing the hypothesis that rind advance rates around an individual clast increase with increasing interfacial curvature.

Oxygen isotope fractionation in the vacuum ultraviolet photodissociation of carbon monoxide: Wavelength, pressure and temperature dependency.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chakraborty, Subrata; Davis, Ryan; Ahmed, Musahid

Several absorption bands exist in the VUV region of Carbon monoxide (CO). Emission spectra indicate that these bands are all predissociative. An experimental investigation of CO photodissociation by vacuum ultraviolet photons (90 to 108 nm; ~13 to 11 eV) from the Advanced Light Source Synchrotron and direct measurement of the associated oxygen isotopic composition of the products are presented here. A wavelength dependency of the oxygen isotopic composition in the photodissociation product was observed. Slope values (δ'{sup 18}O/ δ'{sup 17}O) ranging from 0.76 to 1.32 were observed in oxygen three-isotope space (δ'{sup 18}O vs. δ'{sup 17}O) which correlated with increasingmore » synchrotron photon energy, and indicate a dependency of the upper electronic state specific dissociation dynamics (e.g., perturbation and coupling associated with a particular state). An unprecedented magnitude in isotope separation was observed for photodissociation at the 105 and 107 nm synchrotron bands and are found to be associated with accidental predissociation of the vibrational states ({nu} = 0 and 1) of the upper electronic state E{sup 1}Π. For each synchrotron band, a large (few hundred per mil) extent of isotopic fractionation was observed and the range of fractionation is a combination of column density and exposure time. A significant temperature dependency in oxygen isotopic fractionation was observed, indicating a rotational level dependency in the predissociation process.« less

New insight from noble gas and stable isotopes of geothermal/hydrothermal fluids at Caviahue-Copahue Volcanic Complex: Boiling steam separation and water-rock interaction at shallow depth

NASA Astrophysics Data System (ADS)

Roulleau, Emilie; Tardani, Daniele; Sano, Yuji; Takahata, Naoto; Vinet, Nicolas; Bravo, Francisco; Muñoz, Carlos; Sanchez, Juan

2016-12-01

We measured noble gas and stable isotopes of the geothermal and hydrothermal fluids of the Caviahue-Copahue Volcanic Complex (CCVC), one of the most important geothermal systems in Argentina/Chile, in order to provide new insights into fluid circulation and origin. With the exception of Anfiteatro and Chancho-co geothermal systems, mantle-derived helium dominates in the CCVC fluids, with measured 3He/4He ratios up to 7.86Ra in 2015. Their positive δ15N is an evidence for subducted sediment-derived nitrogen, which is commonly observed in subduction settings. Both He-N2-Ar composition and positive correlation between δD-H2O and δ18O-H2O suggest that the fluids from Anfiteatro and Chancho-co (and partly from Pucon-Mahuida as well, on the southern flank of Copahue volcano) represent a meteoric water composition with a minor magmatic contribution. The Ne, Kr and Xe isotopic compositions are entirely of atmospheric origin, but processes of boiling and steam separation have led to fractionation of their elemental abundances. We modeled the CCVC fluid evolution using Rayleigh distillation curves, considering an initial air saturated geothermal water (ASGW) end-member at 250 and 300 °C, followed by boiling and steam separation at lower temperatures (from 200 °C to 150 °C). Between 2014 and 2015, the CCVC hydrogen and oxygen isotopes shifted from local meteoric water-dominated to andesitic water-dominated signature. This shift is associated with an increase of δ13C values and Stotal, HCl and He contents. These characteristics are consistent with a change in the gas ascent pathway between 2014 and 2015, which in turn induced higher magmatic-hydrothermal contribution in the fluid signature. The composition of the magmatic source of the CCVC fluids is: 3He/4He = 7.7Ra, δ15N = + 6‰, and δ13C = - 6.5‰. Mixing models between air-corrected He and N suggest the involvement of 0.5% to 5% of subducted sediments in the magmatic source. The magmatic sulfur isotopic

Method for isotopic analysis of chlorinated organic compounds

DOEpatents

Holt, Ben D.; Sturchio, Neil C.

1999-01-01

The present invention provides a method for preparing a VOC sample for carbon and chlorine isotope ratio analysis by mass spectrometer. A VOC sample is placed in a combustion tube and reacted with CuO to form CO.sub.2 and CuCl. The CO.sub.2 is then extracted and analyzed for the carbon isotope ratio. The CuCl is separated from the excess CuO and reacted with CH.sub.3 I to form CH.sub.3 Cl, extracted and analyzed for chlorine isotope ratio.

Stable-isotope customer list and summary of shipments, FY 1982

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davis, W.C.

1983-04-01

This compilation is published as an aid to those concerned with the separation and sale of stable isotopes. The inforamtion is divided into four sections: (1) alphabetical list of domestic and foreign customers, showing the stable isotopes purchased during the fiscal year; (2) alphabetical list of isotopes, cross-referenced to customer numbers and divided into domestic and foreign categories; (3) alphabetical list of states and countries, cross-referenced to customer numbers and indicating geographical concentrations of isotope users; and (4) tabulation of the shipments, quantities, and dollars for domestic, foreign, and project categories for each isotope.

Mass fractionation processes of transition metal isotopes

NASA Astrophysics Data System (ADS)

Zhu, X. K.; Guo, Y.; Williams, R. J. P.; O'Nions, R. K.; Matthews, A.; Belshaw, N. S.; Canters, G. W.; de Waal, E. C.; Weser, U.; Burgess, B. K.; Salvato, B.

2002-06-01

Recent advances in mass spectrometry make it possible to utilise isotope variations of transition metals to address some important issues in solar system and biological sciences. Realisation of the potential offered by these new isotope systems however requires an adequate understanding of the factors controlling their isotope fractionation. Here we show the results of a broadly based study on copper and iron isotope fractionation during various inorganic and biological processes. These results demonstrate that: (1) naturally occurring inorganic processes can fractionate Fe isotope to a detectable level even at temperature ˜1000°C, which challenges the previous view that Fe isotope variations in natural system are unique biosignatures; (2) multiple-step equilibrium processes at low temperatures may cause large mass fractionation of transition metal isotopes even when the fractionation per single step is small; (3) oxidation-reduction is an importation controlling factor of isotope fractionation of transition metal elements with multiple valences, which opens a wide range of applications of these new isotope systems, ranging from metal-silicate fractionation in the solar system to uptake pathways of these elements in biological systems; (4) organisms incorporate lighter isotopes of transition metals preferentially, and transition metal isotope fractionation occurs stepwise along their pathways within biological systems during their uptake.

Metal stable isotopes in low-temperature systems: A primer

USGS Publications Warehouse

Bullen, T.D.; Eisenhauer, A.

2009-01-01

Recent advances in mass spectrometry have allowed isotope scientists to precisely determine stable isotope variations in the metallic elements. Biologically infl uenced and truly inorganic isotope fractionation processes have been demonstrated over the mass range of metals. This Elements issue provides an overview of the application of metal stable isotopes to low-temperature systems, which extend across the borders of several science disciplines: geology, hydrology, biology, environmental science, and biomedicine. Information on instrumentation, fractionation processes, data-reporting terminology, and reference materials presented here will help the reader to better understand this rapidly evolving field.

The fusion of advanced fuels to produce medical isotopes using inertial electrostatic confinement

NASA Astrophysics Data System (ADS)

Cipiti, Benjamin B.

Experiments are described that used an Inertial Electrostatic Confinement (IEC) fusion device to create radioisotopes for medical diagnostics. The IEC concept utilizes spherically concentric electrodes to accelerate fusion ions to high energies, allowing the use of the D-D and advanced D-3He fusion reactions. The D-3He reaction produces a high-energy 14.7 MeV proton, and this proton is energetic enough to be used to create radioisotopes. This dissertation focuses first on where specifically the fusion reactions are occurring in the IEC device. It was found that at 2 mtorr operating pressures, 70% of the D-D reactions occur throughout the entire volume of the vacuum chamber. About 22% of the reactions occur in a small core in the center of the device, and the other 8% are due to embedded D-D reactions in the cathode of the device. On the other hand, for D-3He, 95% of the reactions are due to embedded reactions, and the other 5% come from a small core in the center of the device. Beam-target D-3He fusion was used to create medical isotopes in two different systems. The designs focused on creating short-lived species capable of use in Positron Emission Tomography. The first isotope created was 94mTc, a positron emitter with a 52-minute half-life. Approximately 1.5 nCi of 94mTc were created using the 94Mo(p,n) 94mTc reaction. The second isotope created was 13N, a positron emitter with a ten-minute half-life. Approximately 1.0 nCi of 13N was created using the 16O(p,alpha)13N reaction. The final part of the research investigated the effects of deuterium and helium implantation in the tungsten-rhenium cathode of the IEC device. The effect of the implantation on the surface morphology of pure tungsten was also determined using scanning electron microscopy. Deuterium did not appear to affect the surface of tungsten after high temperature (>800 C) implantation. Helium created a porous surface structure at the same temperatures starting at about 4 x 1016 ions/cm2. The pores

Attomole quantitation of protein separations with accelerator mass spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vogel, J S; Grant, P G; Buccholz, B A

2000-12-15

Quantification of specific proteins depends on separation by chromatography or electrophoresis followed by chemical detection schemes such as staining and fluorophore adhesion. Chemical exchange of short-lived isotopes, particularly sulfur, is also prevalent despite the inconveniences of counting radioactivity. Physical methods based on isotopic and elemental analyses offer highly sensitive protein quantitation that has linear response over wide dynamic ranges and is independent of protein conformation. Accelerator mass spectrometry quantifies long-lived isotopes such as 14C to sub-attomole sensitivity. We quantified protein interactions with small molecules such as toxins, vitamins, and natural biochemicals at precisions of 1-5% . Micro-proton-induced-xray-emission quantifies elemental abundancesmore » in separated metalloprotein samples to nanogram amounts and is capable of quantifying phosphorylated loci in gels. Accelerator-based quantitation is a possible tool for quantifying the genome translation into proteome.« less

DANCEing with the Stars: Measuring Neutron Capture on Unstable Isotopes with DANCE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Couture, A.; Bond, E.; Bredeweg, T. A.

2009-03-10

Isotopes heavier than iron are known to be produced in stars through neutron capture processes. Two major processes, the slow (s) and rapid (r) processes are each responsible for 50% of the abundances of the heavy isotopes. The neutron capture cross sections of the isotopes on the s process path reveal information about the expected abundances of the elements as well as stellar conditions and dynamics. Until recently, measurements on unstable isotopes, which are most important for determining stellar temperatures and reaction flow, have not been experimentally feasible. The Detector for Advance Neutron Capture Experiments (DANCE) located at the Losmore » Alamos Neutron Science Center (LANSCE) was designed to perform time-of-flight neutron capture measurements on unstable isotopes for nuclear astrophysics, stockpile stewardship, and reactor development. DANCE is a 4-{pi}BaF{sub 2} scintillator array which can perform measurements on sub-milligram samples of isotopes with half-lives as short as a few hundred days. These cross sections are critical for advancing our understanding of the production of the heavy isotopes.« less

Boundary-value problem for a counterrotating electrical discharge in an axial magnetic field. [plasma centrifuge for isotope separation

NASA Technical Reports Server (NTRS)

Hong, S. H.; Wilhelm, H. E.

1978-01-01

An electrical discharge between two ring electrodes embedded in the mantle of a cylindrical chamber is considered, in which the plasma in the anode and cathode regions rotates in opposite directions under the influence of an external axial magnetic field. The associated boundary-value problem for the coupled partial differential equations describing the azimuthal velocity and radial current-density fields is solved in closed form. The velocity, current density, induced magnetic induction, and electric fields are presented for typical Hartmann numbers, magnetic Reynolds numbers, and geometry parameters. The discharge is shown to produce anodic and cathodic plasma sections rotating at speeds of the order 1,000,000 cm/sec for conventional magnetic field intensities. Possible application of the magnetoactive discharge as a plasma centrifuge for isotope separation is discussed.

Isotopic Evidence of Unaccounted for Fe and Cu Erythropoietic Pathways

NASA Astrophysics Data System (ADS)

Albarede, F.; Telouk, P.; Lamboux, A.; Jaouen, K.; Balter, V.

2011-12-01

Despite its potential importance for understanding perturbations in the Fe-Cu homeostatic pathways, the natural isotopic variability of these metals in the human body remains unexplored. We measured the Fe, Cu, and Zn isotope compositions of total blood, serum, and red blood cells of ~50 young blood donors by multiple-collector ICP-MS after separation and purification by anion exchange chromatography. Zn is on average 0.2 permil heavier in erythrocytes (δ 66Zn=0.44±0.33 permil) with respect to serum but shows much less overall isotopic variability than Fe and Cu, which indicates that isotope fractionation depends more on redox conditions than on ligand coordination. On average, Fe in erythrocytes (δ 56Fe=-2.59±0.47 permil) is isotopically light by 1-2 permil with respect to serum, whereas Cu in erythrocytes (δ 65Cu=0.56±0.50 permil) is 0.8 percent heavier. Fe and Cu isotope compositions clearly separate erythrocytes of men and women. Fe and Cu from B-type men erythrocytes are visibly more fractionated than all the other blood types. Isotope compositions provide an original method for evaluating metal mass balance and homeostasis. Natural isotope variability shows that the current models of Fe and Cu erythropoiesis, which assume that erythropoiesis is restricted to bone marrow, violate mass balance requirements. It unveils unsuspected major pathways for Fe, with erythropoietic production of isotopically heavy ferritin and hemosiderin, and for Cu, with isotopically light Cu being largely channeled into blood and lymphatic circulation rather than into superoxide dismutase-laden erythrocytes. Iron isotopes provide an intrinsic measuring rod of the erythropoietic yield, while Cu isotopes seem to gauge the relative activity of erythropoiesis and lymphatics.

Compelling Research Opportunities using Isotopes

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

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 andmore » 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

High Throughput Strontium Isotope Method for Monitoring Fluid Flow Related to Geological CO2 Storage

NASA Astrophysics Data System (ADS)

Capo, R. C.; Wall, A. J.; Stewart, B. W.; Phan, T. T.; Jain, J. C.; Hakala, J. A.; Guthrie, G. D.

2012-12-01

Natural isotope tracers, such as strontium (Sr), can be a unique and powerful component of a monitoring strategy at a CO2 storage site, facilitating both the quantification of reaction progress for fluid-rock interactions and the tracking of brine migration caused by CO2 injection. Several challenges must be overcome, however, to enable the routine use of isotopic tracers, including the ability to rapidly analyze numerous aqueous samples with potentially complex chemical compositions. In a field situation, it might be necessary to analyze tens of samples over a short period of time to identify subsurface reactions and respond to unexpected fluid movement in the host formation. These conditions require streamlined Sr separation chemistry for samples ranging from pristine groundwaters to those containing high total dissolved solids, followed by rapid measurement of isotope ratios with high analytical precision. We have optimized Sr separation chemistry and MC-ICP-MS methods to provide rapid and precise measurements of isotope ratios in geologic, hydrologic, and environmental samples. These improvements will allow an operator to independently prepare samples for Sr isotope analysis off-site using fast, low cost chemical separation procedures and commercially available components. Existing vacuum-assisted Sr separation procedures were modified by using inexpensive disposable parts to eliminate cross contamination. Experimental results indicate that the modified columns provide excellent separation of Sr from chemically complex samples and that Sr can be effectively isolated from problematic matrix elements (e.g., Ca, Ba, K) associated with oilfield brines and formation waters. The separation procedure is designed for high sample throughput in which batches of 24 samples can be processed in approximately 2 hours, and are ready for Sr isotope measurements by MC-ICP-MS immediately after collection from the columns. Precise Sr isotope results can be achieved by MC

ANITA (Advanced Network for Isotope and TArget laboratories) - The urgent need for a European target preparation network

NASA Astrophysics Data System (ADS)

Schumann, Dorothea; Sibbens, Goedele; Stolarz, Anna; Eberhardt, Klaus; Lommel, Bettina; Stodel, Christelle

2018-05-01

A wide number of research fields in the nuclear sector requires high-quality and well-characterized samples and targets. Currently, only a few laboratories own or have access to the equipment allowing fulfilling such demands. Coordination of activities and sharing resources is therefore mandatory to meet the increasing needs. This very urgent issue has now been addressed by six European target laboratories with an initiative called ANITA (Advanced Network for Isotope and TArget laboratories). The global aim of ANITA is to establish an overarching research infrastructure service for isotope and target production and develop a tight cooperation between the target laboratories in Europe in order to transfer the knowledge and improve the production techniques of well-characterized samples and targets. Moreover, the interaction of the target producers with the users shall be encouraged and intensified to deliver tailor-made targets best-suited to the envisaged experiments. For the realization of this ambitious goal, efforts within the European Commission and strong support by the target-using communities will be necessary. In particular, an appropriate funding instrument has to be found and applied, enabling ANITA to develop from an initiative employed by the interested parties to a real coordination platform.

Method for isotopic analysis of chlorinated organic compounds

DOEpatents

Holt, B.D.; Sturchio, N.C.

1999-08-24

The present invention provides a method for preparing a VOC sample for carbon and chlorine isotope ratio analysis by mass spectrometer. A VOC sample is placed in a combustion tube and reacted with CuO to form CO{sub 2} and CuCl. The CO{sub 2} is then extracted and analyzed for the carbon isotope ratio. The CuCl is separated from the excess CuO and reacted with CH{sub 3}I to form CH{sub 3}Cl, extracted and analyzed for chlorine isotope ratio. 9 figs.

Integrating isotopic fingerprinting with petrology: how do igneous rocks evolve?

NASA Astrophysics Data System (ADS)

Davidson, J. P.

2002-12-01

In the title of his seminal work, N.L. Bowen recognized the fundamental importance of magmatic evolution in producing the spectrum of igneous rocks. Indeed it is difficult to imagine a hot highly reactive fluid passing through c. 100 km of a chemically distinct medium (lithosphere) without evolving through cooling, crystallization and interaction with the wall rocks. The fact that magmas evolve - almost invariably through open system processes - has been largely marginalized in the past 30 years by the desire to use them as probes of mantle source regions. This perspective has been driven principally by advances offered by isotope geochemistry, through which components and sources can be effectively fingerprinted. Two fundamental observations urge caution in ignoring differentiation effects; 1) the scarcity of truly primary magmas according to geochemical criteria (recognized long ago by petrologists), and 2) the common occurrence of petrographic criteria attesting to open system evolution. Recent advances in multicollector mass spectrometry permit integration of the powerful diagnostic tools of isotope geochemistry with petrographic observations through accurate and precise analysis of small samples. Laser ablation and microdrilling enable sampling within and between mineral phases. The results of our microsampling investigations give widespread support for open system evolution of magmas, and provide insights into the mechanisms and timescales over which this occurs. For example; 1) core-rim decreases in 87Sr/86Sr in zoned plagioclase crystals from 1982 lavas of El Chichon volcano, Mexico, argue that the zoning and isotopic changes are in response to magma recharge mixing with an originally contaminated resident magma; 2) Single grain and intra-grain isotopic analyses of mineral phases from Ngauruhoe andesites (New Zealand) are highly variable, arguing that bulk rock data reflect mechanical aggregations of components which have evolved in discrete domains of the

Constraints on post-depositional isotope modifications in East Antarctic firn from analysing temporal changes of isotope profiles

NASA Astrophysics Data System (ADS)

Münch, Thomas; Kipfstuhl, Sepp; Freitag, Johannes; Meyer, Hanno; Laepple, Thomas

2017-09-01

The isotopic composition of water in ice sheets is extensively used to infer past climate changes. In low-accumulation regions their interpretation is, however, challenged by poorly constrained effects that may influence the initial isotope signal during and after deposition of the snow. This is reflected in snow-pit isotope data from Kohnen Station, Antarctica, which exhibit a seasonal cycle but also strong interannual variations that contradict local temperature observations. These inconsistencies persist even after averaging many profiles and are thus not explained by local stratigraphic noise. Previous studies have suggested that post-depositional processes may significantly influence the isotopic composition of East Antarctic firn. Here, we investigate the importance of post-depositional processes within the open-porous firn (≳ 10 cm depth) at Kohnen Station by separating spatial from temporal variability. To this end, we analyse 22 isotope profiles obtained from two snow trenches and examine the temporal isotope modifications by comparing the new data with published trench data extracted 2 years earlier. The initial isotope profiles undergo changes over time due to downward advection, firn diffusion and densification in magnitudes consistent with independent estimates. Beyond that, we find further modifications of the original isotope record to be unlikely or small in magnitude (≪ 1 ‰ RMSD). These results show that the discrepancy between local temperatures and isotopes most likely originates from spatially coherent processes prior to or during deposition, such as precipitation intermittency or systematic isotope modifications acting on drifting or loose surface snow.

Recent advances in understanding atmospheric CO based on stable isotope measurements

NASA Astrophysics Data System (ADS)

Popa, Maria Elena; Naus, Stijn; Ferrero Lopez, Noelia; Vijverberg, Sem; de Leeuw, Selma; Röckmann, Thomas

2017-04-01

Carbon monoxide (CO) plays an important role for atmospheric chemistry and for carbon cycling in the atmosphere. Via its reaction with the OH radical it influences concentrations of many other trace gases, it is an important precursor for O3 formation, and its oxidation leads to the formation of about 1 Pg C per year of CO2. The natural and anthropogenic sources of CO are subject to relatively large temporal changes due to natural variability (e.g. biomass burning), industrial activity and mitigation measures (e.g. fossil fuel burning), variations in precursor compounds (e.g. CH4 and VOC) and variations in the abundance of the OH radical in the atmosphere, which are difficult to quantify. Isotope measurements can be used to distinguish between the effects of individual sources and sinks to put tighter constrains on its budget, but the isotopic characterization of the CO sources is in many cases still based on a few relatively old measurements that did not allow to account for dependence on parameters. We will present an update of the isotopic composition of several sources and removal processes of CO that have been carried out in the past years with the automated continuous-flow IRMS system at Utrecht University. This includes: - the previously unknown isotopic composition of direct biogenic CO emissions - a surprisingly large variability in the isotopic composition of CO emitted by different vehicles and single vehicles under various driving conditions - previously very poorly investigated signatures, like the fractionation in the removal of CO by soils, and its interaction with CO that is simultaneously emitted from soil. These results from process specific investigations will be linked to recent atmospheric measurements at various locations.

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...

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 ...

A preliminary study for the production of high specific activity radionuclides for nuclear medicine obtained with the isotope separation on line technique.

PubMed

Borgna, F; Ballan, M; Corradetti, S; Vettorato, E; Monetti, A; Rossignoli, M; Manzolaro, M; Scarpa, D; Mazzi, U; Realdon, N; Andrighetto, A

2017-09-01

Radiopharmaceuticals represent a fundamental tool for nuclear medicine procedures, both for diagnostic and therapeutic purposes. The present work aims to explore the Isotope Separation On-Line (ISOL) technique for the production of carrier-free radionuclides for nuclear medicine at SPES, a nuclear physics facility under construction at INFN-LNL. Stable ion beams of strontium, yttrium and iodine were produced using the SPES test bench (Front-End) to simulate the production of 89 Sr, 90 Y, 125 I and 131 I and collected with good efficiency on suitable targets. Copyright © 2017 Elsevier Ltd. All rights reserved.

Sr isotopic tracer study of the Samail ophiolite, Oman.

USGS Publications Warehouse

Lanphere, M.A.; Coleman, R.G.; Hopson, C.A.

1981-01-01

Rb and Sr concentrations and Sr-isotopic compositions were measured in 41 whole-rock samples and 12 mineral separates from units of the Samail ophiolite, including peridotite, gabbro, plagiogranite, diabase dykes, and gabbro and websterite dykes within the metamorphic peridotite. Ten samples of cumulate gabbro from the Wadir Kadir section and nine samples from the Wadi Khafifah section have 87Sr/86Sr ratios of 0.70314 + or - 0.00030 and 0.70306 + or - 0.00034, respectively. The dispersion in Sr- isotopic composition may reflect real heterogeneities in the magma source region. The average Sr-isotopic composition of cumulate gabbro falls in the range of isotopic compositions of modern MORB. The 87Sr/86Sr ratios of noncumulate gabbro, plagiogranite, and diabase dykes range 0.7034-0.7047, 0.7038-0.7046 and 0.7037- 0.7061, respectively. These higher 87Sr/86Sr ratios are due to alteration of initial magmatic compositions by hydrothermal exchange with sea-water. Mineral separates from dykes that cut harzburgite tectonite have Sr-isotopic compositions which agree with that of cumulate gabbro. These data indicate that the cumulate gabbro and the different dykes were derived from partial melting of source regions that had similar long-term histories and chemical compositions.-T.R.

Measurement of plutonium isotope ratios in nuclear fuel samples by HPLC-MC-ICP-MS

NASA Astrophysics Data System (ADS)

Günther-Leopold, I.; Waldis, J. Kobler; Wernli, B.; Kopajtic, Z.

2005-04-01

Radioactive isotopes are traditionally quantified by means of radioactivity counting techniques ([alpha], [beta], [gamma]). However, these methods often require extensive matrix separation and sample purification before the identification of specific isotopes and their relative abundance is possible as it is necessary in the frame of post-irradiation examinations on nuclear fuel samples. The technique of multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS) is attracting much attention because it permits the precise measurement of the isotope compositions for a wide range of elements combined with excellent limits of detection due to high ionization efficiencies. The present paper describes one of the first applications of an online high-performance liquid chromatographic separation system coupled to a MC-ICP-MS in order to overcome isobaric interferences for the determination of the plutonium isotope composition and concentrations in irradiated nuclear fuels. The described chromatographic separation is sufficient to prevent any isobaric interference between 238Pu present at trace concentrations and 238U present as the main component of the fuel samples. The external reproducibility of the uncorrected plutonium isotope ratios was determined to be between 0.04 and 0.2% (2 s) resulting in a precision in the [per mille sign] range for the isotopic vectors of the irradiated fuel samples.

Dissolution of barite for the analysis of strontium isotopes and other chemical and isotopic variations using aqueous sodium carbonate

USGS Publications Warehouse

Breit, G.N.; Simmons, E.C.; Goldhaber, M.B.

1985-01-01

A simple procedure for preparing barite samples for chemical and isotopic analysis is described. Sulfate ion, in barite, in the presence of high concentrations of aqueous sodium carbonate, is replaced by carbonate. This replacement forms insoluble carbonates with the cations commonly in barite: Ba, Sr, Ca and Pb. Sulfate is released into the solution by the carbonate replacement and is separated by filtration. The aqueous sulfate can then be reprecipitated for analysis of the sulfur and oxygen isotopes. The cations in the carbonate phase can be dissolved by acidifying the solid residue. Sr can be separated from the solution for Sr isotope analysis by ion-exchange chromatography. The sodium carbonate used contains amounts of Sr which will affect almost all barite 87Sr 86Sr ratios by less than 0.00001 at 1.95?? of the mean. The procedure is preferred over other techniques used for preparing barite samples for the determination of 87Sr 86Sr ratios because it is simple, rapid and enables simultaneous determination of many compositional parameters on the same material. ?? 1985.

Optimization and comparison of simultaneous and separate acquisition protocols for dual isotope myocardial perfusion SPECT.

PubMed

Ghaly, Michael; Links, Jonathan M; Frey, Eric C

2015-07-07

Dual-isotope simultaneous-acquisition (DISA) rest-stress myocardial perfusion SPECT (MPS) protocols offer a number of advantages over separate acquisition. However, crosstalk contamination due to scatter in the patient and interactions in the collimator degrade image quality. Compensation can reduce the effects of crosstalk, but does not entirely eliminate image degradations. Optimizing acquisition parameters could further reduce the impact of crosstalk. In this paper we investigate the optimization of the rest Tl-201 energy window width and relative injected activities using the ideal observer (IO), a realistic digital phantom population and Monte Carlo (MC) simulated Tc-99m and Tl-201 projections as a means to improve image quality. We compared performance on a perfusion defect detection task for Tl-201 acquisition energy window widths varying from 4 to 40 keV centered at 72 keV for a camera with a 9% energy resolution. We also investigated 7 different relative injected activities, defined as the ratio of Tc-99m and Tl-201 activities, while keeping the total effective dose constant at 13.5 mSv. For each energy window and relative injected activity, we computed the IO test statistics using a Markov chain Monte Carlo (MCMC) method for an ensemble of 1,620 triplets of fixed and reversible defect-present, and defect-absent noisy images modeling realistic background variations. The volume under the 3-class receiver operating characteristic (ROC) surface (VUS) was estimated and served as the figure of merit. For simultaneous acquisition, the IO suggested that relative Tc-to-Tl injected activity ratios of 2.6-5 and acquisition energy window widths of 16-22% were optimal. For separate acquisition, we observed a broad range of optimal relative injected activities from 2.6 to 12.1 and acquisition energy window of widths 16-22%. A negative correlation between Tl-201 injected activity and the width of the Tl-201 energy window was observed in these ranges. The results

Optimization and comparison of simultaneous and separate acquisition protocols for dual isotope myocardial perfusion SPECT

PubMed Central

Ghaly, Michael; Links, Jonathan M; Frey, Eric C

2015-01-01

Dual-isotope simultaneous-acquisition (DISA) rest-stress myocardial perfusion SPECT (MPS) protocols offer a number of advantages over separate acquisition. However, crosstalk contamination due to scatter in the patient and interactions in the collimator degrade image quality. Compensation can reduce the effects of crosstalk, but does not entirely eliminate image degradations. Optimizing acquisition parameters could further reduce the impact of crosstalk. In this paper we investigate the optimization of the rest Tl-201 energy window width and relative injected activities using the ideal observer (IO), a realistic digital phantom population and Monte Carlo (MC) simulated Tc-99m and Tl-201 projections as a means to improve image quality. We compared performance on a perfusion defect detection task for Tl-201 acquisition energy window widths varying from 4 to 40 keV centered at 72 keV for a camera with a 9% energy resolution. We also investigated 7 different relative injected activities, defined as the ratio of Tc-99m and Tl-201 activities, while keeping the total effective dose constant at 13.5 mSv. For each energy window and relative injected activity, we computed the IO test statistics using a Markov chain Monte Carlo (MCMC) method for an ensemble of 1,620 triplets of fixed and reversible defect-present, and defect-absent noisy images modeling realistic background variations. The volume under the 3-class receiver operating characteristic (ROC) surface (VUS) was estimated and served as the figure of merit. For simultaneous acquisition, the IO suggested that relative Tc-to-Tl injected activity ratios of 2.6–5 and acquisition energy window widths of 16–22% were optimal. For separate acquisition, we observed a broad range of optimal relative injected activities from 2.6 to 12.1 and acquisition energy window of widths 16–22%. A negative correlation between Tl-201 injected activity and the width of the Tl-201 energy window was observed in these ranges. The results

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)

Steroid isotopic standards for gas chromatography-combustion isotope ratio mass spectrometry (GCC-IRMS).

PubMed

Zhang, Ying; Tobias, Herbert J; Brenna, J Thomas

2009-03-01

Carbon isotope ratio (CIR) analysis of urinary steroids using gas chromatography-combustion isotope ratio mass spectrometry (GCC-IRMS) is a recognized test to detect illicit doping with synthetic testosterone. There are currently no universally used steroid isotopic standards (SIS). We adapted a protocol to prepare isotopically uniform steroids for use as a calibrant in GCC-IRMS that can be analyzed under the same conditions as used for steroids extracted from urine. Two separate SIS containing a mixture of steroids were created and coded CU/USADA 33-1 and CU/USADA 34-1, containing acetates and native steroids, respectively. CU/USADA 33-1 contains 5alpha-androstan-3beta-ol acetate (5alpha-A-AC), 5alpha-androstan-3alpha-ol-17-one acetate (androsterone acetate, A-AC), 5beta-androstan-3alpha-ol-11, 17-dione acetate (11-ketoetiocholanolone acetate, 11k-AC) and 5alpha-cholestane (Cne). CU/USADA 34-1 contains 5beta-androstan-3alpha-ol-17-one (etiocholanolone, E), 5alpha-androstan-3alpha-ol-17-one (androsterone, A), and 5beta-pregnane-3alpha, 20alpha-diol (5betaP). Each mixture was prepared and dispensed into a set of about 100 ampoules using a protocol carefully designed to minimize isotopic fractionation and contamination. A natural gas reference material, NIST RM 8559, traceable to the international standard Vienna PeeDee Belemnite (VPDB) was used to calibrate the SIS. Absolute delta(13)C(VPDB) and Deltadelta(13)C(VPDB) values from randomly selected ampoules from both SIS indicate uniformity of steroid isotopic composition within measurement reproducibility, SD(delta(13)C)<0.2 per thousand. This procedure for creation of isotopic steroid mixtures results in consistent standards with isotope ratios traceable to the relevant international reference material.

Interactions between surface waters in King George Island, Antarctica - a stable isotope perspective

NASA Astrophysics Data System (ADS)

Perşoiu, Aurel; Bădăluşă, Carmen

2017-04-01

In this paper we present a first study of the isotopic composition of surface waters in the southern peninsulas (Barton, Fildes, Weaver and Potter) of King George Island, Antarctica. We have collected > 200 samples of snow and snowmelt, water (lake, river and spring), ice (glacier ice and permafrost) from the four peninsulas in February 2016 and analyzed them for their oxygen and hydrogen stable isotopic composition. Samples from lake water (50+) indicate a clear west-east depletion trend, suggesting a rain-out process as air masses are moving westward (and are progressively depleted in heavy isotopes) from their origin in the Drake Passage. In both Fildes and Barton Peninsulas, permafrost samples have the heaviest isotopic composition, most probably due to preferential incorporation of heavy isotopes in the ice during freezing (and no fractionation during melting). As permafrost melts, the resulting water mixes with isotopically lighter infiltrated snowmelt, and thus the groundwater has a lower isotopic composition. Further, lake and river (the later fed by lakes) water has the lightest isotopic composition, being derived mostly from the melting of light snow and glacier ice. It seems feasible to separate isotopically water in lakes/rivers (largely fed by melting multi-year glaciers and snow) and water from melting of snow/ground ice This preliminary study suggests that it is possible to separate various water sources in the southern peninsulas of King George Island, and this separation could be used to study permafrost degradation, as well as feeding and migration patterns in the bird fauna, with implications for protection purposes. Acknowledgments. The National Institute of Research and Development for Biological Sciences (Bucharest, Romania) and the Korean polar institute financially supported fieldwork in King George Island. We thank the personal at King Sejong (South Korea), Belingshaussen (Russia) and Carlini (Argentina) stations in King George Island for

Advanced fire-resistant forms of activated carbon and methods of adsorbing and separating gases using same

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xiong, Yongliang; Wang, Yifeng

Advanced, fire-resistant activated carbon compositions useful in adsorbing gases; and having vastly improved fire resistance are provided, and methods for synthesizing the compositions are also provided. The advanced compositions have high gas adsorption capacities and rapid adsorption kinetics (comparable to commercially-available activated carbon), without having any intrinsic fire hazard. They also have superior performance to Mordenites in both adsorption capacities and kinetics. In addition, the advanced compositions do not pose the fibrous inhalation hazard that exists with use of Mordenites. The fire-resistant compositions combine activated carbon mixed with one or more hydrated and/or carbonate-containing minerals that release H.sub.2O and/or CO.sub.2more » when heated. This effect raises the spontaneous ignition temperature to over 500.degree. C. in most examples, and over 800.degree. C. in some examples. Also provided are methods for removing and/or separating target gases, such as Krypton or Argon, from a gas stream by using such advanced activated carbons.« less

Copper and Zinc isotope composition of CR, CB and CH-like meteorites.

NASA Astrophysics Data System (ADS)

Russell, S.; Zhu, X.; Guo, Y.; Mullane, E.; Gounelle, M.; Mason, T.; Coles, B.

2003-04-01

Copper and zinc isotopes have recently been shown to be variable in isotopic composi-tion among terrestrial and extraterrestrial materials [1-3]. For this study, we have se-lected samples (bulk meteorite and chondrule separates) from the CR meteorite clan: Bencubbin (CB), Renazzo (CR2), NWA 801 (CR2), and HaH237 (CH-like). These meteorites were selected because meteorites from this clan have experienced very little alteration since their initial formation [4] and for their extremely high refrac-tory/volatile element ratios. The latter characteristic may allow a test of the correlation observed by [2] between element ratios and Cu isotope composition. Measurements were performed on NHM/IC Micromass Isoprobe and Oxford Nu MC-ICP-MS using techniques described elsewhere [1,5]. Each of the meteorites measured so far for Cu and Zn are isotopically light compared to the terrestrial mantle. This suggests that the terrestrial value may have been altered from the pristine solar system value, or else there were multiple early solar system components. Zinc isotopic com-positions lie on a fractionation line and range from δ66ZnNIST = -1.4±0.1ppm (bulk NWA801) to -1.9±0.1ppm (separated chondrule, NWA 801). Copper isotope compositions vary from δ65CuNIST976 = -1.5±0.1ppm (bulk Renazzo) to -3.1±0.1ppm (separated chondrule, NWA 801). Two chondrules from NWA 801 have differing Cu isotope values (-3.1±0.1 and -2.0±0.1ppm) and both are lighter than the bulk meteorite (-1.9±0.1ppm), suggesting a lack of equilibration with respect to Cu in this meteorite. The light values for the two separated chondrules, compared the bulk meteorite, hints that chondrules may be isotopically lighter than co-existing matrix, metal and sulphides with respect to Cu. The copper isotope compositions are not as isotopically light as expected for the high refractory/volatile element ratio observed in these chondrites. Thus a model to account for the Cu isotopes in chondrites may require greater com

Cs-Ba separation using N 2O as a reactant gas in a Multiple Collector-Inductively Coupled Plasma Mass Spectrometer collision-reaction cell: Application to the measurements of Cs isotopes in spent nuclear fuel samples

NASA Astrophysics Data System (ADS)

Granet, M.; Nonell, A.; Favre, G.; Chartier, F.; Isnard, H.; Moureau, J.; Caussignac, C.; Tran, B.

2008-11-01

In the general frameworks of the nuclear fuel cycle and environmental research field, the Cs isotopic composition must be known with high precision and accuracy. The direct determination of Cs isotopes by mass spectrometry techniques is generally hampered by the presence of Ba isobaric interferences however. Here we present a new method which takes advantage of the collision-reaction cell based Multiple Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICPMS) and allows to analyse Cs isotopes in the presence of Ba without prior separation step. The addition of N 2O gas in the cell leads to an antagonistic behavior of Cs + and Ba + as the latter reacts with the gas to form BaO + and BaOH + products whereas Cs + remains unreactive. The efficiency of the method was demonstrated for an UOx sample by comparing the results obtained (1) from the measurements of pure Cs fractions and (2) from Fission Products fractions containing more than 30 ionisable elements in addition to Cs, Ba, and where U and Pu were previously removed by using ion exchange resin. An excellent agreement is achieved between each set of experiments with an external reproducibility always better than 0.5% (RSD, k = 2). This study confirms the strong potential of collision-reaction cell to measure Cs isotopes in presence of interfering Ba, precluding therefore former systematic chemical separations.

Isotope effects on the optical spectra of semiconductors

NASA Astrophysics Data System (ADS)

Cardona, Manuel; Thewalt, M. L. W.

2005-10-01

Since the end of the cold war, macroscopic amounts of separated stable isotopes of most elements have been available “off the shelf” at affordable prices. Using these materials, single crystals of many semiconductors have been grown and the dependence of their physical properties on isotopic composition has been investigated. The most conspicuous effects observed have to do with the dependence of phonon frequencies and linewidths on isotopic composition. These affect the electronic properties of solids through the mechanism of electron-phonon interaction, in particular, in the corresponding optical excitation spectra and energy gaps. This review contains a brief introduction to the history, availability, and characterization of stable isotopes, including their many applications in science and technology. It is followed by a concise discussion of the effects of isotopic composition on the vibrational spectra, including the influence of average isotopic masses and isotopic disorder on the phonons. The final sections deal with the effects of electron-phonon interaction on energy gaps, the concomitant effects on the luminescence spectra of free and bound excitons, with particular emphasis on silicon, and the effects of isotopic composition of the host material on the optical transitions between the bound states of hydrogenic impurities.

The influence of kinetics on the oxygen isotope composition of calcium carbonate

NASA Astrophysics Data System (ADS)

Watkins, James M.; Nielsen, Laura C.; Ryerson, Frederick J.; DePaolo, Donald J.

2013-08-01

Paleotemperature reconstructions rely on knowledge of the equilibrium separation of oxygen isotopes between aqueous solution and calcium carbonate. Although oxygen isotope separation is expected on theoretical grounds, the temperature-dependence remains uncertain because other factors, such as slow exchange of isotopes between dissolved CO2-species and water, can obscure the temperature signal. This is problematic for crystal growth experiments on laboratory timescales and for interpreting the oxygen isotope composition of crystals formed in natural settings. We present results from experiments in which inorganic calcite is precipitated in the presence of 0.25 μM dissolved bovine carbonic anhydrase (CA). The presence of dissolved CA accelerates oxygen isotope equilibration between the dissolved carbon species CO2, H2CO3, HCO3-, CO32- and water, thereby eliminating this source of isotopic disequilibrium during calcite growth. The experimental results allow us to isolate, for the first time, kinetic oxygen isotope effects occurring at the calcite-water interface. We present a framework of ion-by-ion growth of calcite that reconciles our new measurements with measurements of natural cave calcites that are the best candidate for having precipitated under near-equilibrium conditions. Our findings suggest that isotopic equilibrium between calcite and water is unlikely to have been established in laboratory experiments or in many natural settings. The use of CA in carbonate precipitation experiments offers new opportunities to refine oxygen isotope-based geothermometers and to interrogate environmental variables other than temperature that influence calcite growth rates.

Advances in natural stable isotope ratio analysis of human hair to determine nutritional and metabolic status.

PubMed

Petzke, Klaus J; Fuller, Benjamin T; Metges, Cornelia C

2010-09-01

We review the literature on the use of stable isotope ratios at natural abundance to reveal information about dietary habits and specific nutrient intakes in human hair protein (keratin) and amino acids. In particular, we examine whether hair isotopic compositions can be used as unbiased biomarkers to provide information about nutritional status, metabolism, and diseases. Although the majority of research on the stable isotope ratio analysis of hair has focused on bulk protein, methods have been recently employed to examine amino acid-specific isotope ratios using gas chromatography or liquid chromatography coupled to an isotope ratio mass spectrometer. The isotopic measurement of amino acids has the potential to answer research questions on amino acid nutrition, metabolism, and disease processes and can contribute to a better understanding of the variations in bulk protein isotope ratio values. First results suggest that stable isotope ratios are promising as unbiased nutritional biomarkers in epidemiological research. However, variations in stable isotope ratios of human hair are also influenced by nutrition-dependent nitrogen balance, and more controlled clinical research is needed to examine these effects in human hair. Stable isotope ratio analysis at natural abundance in human hair protein offers a noninvasive method to reveal information about long-term nutritional exposure to specific nutrients, nutritional habits, and in the diagnostics of diseases leading to nutritional stress and impaired nitrogen balance.

Isotopic Abundances as Tracers of the Processes of Lunar Formation

NASA Astrophysics Data System (ADS)

Pahlevan, K.

2011-12-01

different, if the Moon preferentially forms from the liquid or vapor relative to the Earth, mass-dependent isotopic differences at the planetary scale may arise. The large density contrast between liquid and vapor makes phase separation possible. (3) The precision with which planetary isotopic compositions can be determined has increased such that measurements are sensitive to even small degrees of high-temperature phase separation. Using thermodynamic models of silicate liquids to determine the partial vaporization behavior of the major elements, we will present calculations of isotopic fractionation due to liquid-vapor separation for the elements iron, magnesium, silicon, and oxygen. Improvements in analytical precision have largely settled the question of the source of the lunar material - the Earth's mantle - and isotopic measurements are now beginning to yield insight into the high-temperatures processes operating during lunar formation.

Improvements in Cd stable isotope analysis achieved through use of liquid-liquid extraction to remove organic residues from Cd separates obtained by extraction chromatography.

PubMed

Murphy, Katy; Rehkämper, Mark; Kreissig, Katharina; Coles, Barry; van de Flierdt, Tina

2016-01-23

Organic compounds released from resins that are commonly employed for trace element separations are known to have a detrimental impact on the quality of isotopic analyses by MC-ICP-MS. A recent study highlighted that such effects can be particularly problematic for Cd stable isotope measurements (M. Gault-Ringold and C. H. Stirling, J. Anal. At. Spectrom. , 2012, 27 , 449-459). In this case, the final stage of sample purification commonly applies extraction chromatography with Eichrom TRU resin, which employs particles coated with octylphenyl- N , N -di-isobutyl carbamoylphosphine oxide (CMPO) dissolved in tri- n -butyl phosphate (TBP). During chromatography, it appears that some of these compounds are eluted alongside Cd and cannot be removed by evaporation due to their high boiling points. When aliquots of the zero-ε reference material were processed through the purification procedure, refluxed in concentrated HNO 3 and analyzed at minimum dilution (in 1 ml 0.1 M HNO 3 ), they yielded Cd isotopic compositions (ε 114/110 Cd = 4.6 ± 3.4, 2SD, n = 4) that differed significantly from the expected value, despite the use of a double spike technique to correct for instrumental mass fractionation. This result was accompanied by a 35% reduction in instrumental sensitivity for Cd. With increasing dilution of the organic resin residue, both of these effects are reduced and they are insignificant when the eluted Cd is dissolved in ≥3 ml 0.1 M HNO 3 . Our results, furthermore, indicate that the isotopic artefacts are most likely related to anomalous mass bias behavior. Previous studies have shown that perchloric acid can be effective at avoiding such effects (Gault-Ringold and Stirling, 2012; K. C. Crocket, M. Lambelet, T. van de Flierdt, M. Rehkämper and L. F. Robinson, Chem. Geol. , 2014, 374-375 , 128-140), presumably by oxidizing the resin-derived organics, but there are numerous disadvantages to its use. Here we show that liquid-liquid extraction with n -heptane

Separation processes using expulsion from dilute supercritical solutions

DOEpatents

Cochran, Jr., Henry D.

1993-01-01

A process for separating isotopes as well as other mixtures by utilizing the behavior of dilute repulsive or weakly attractive elements of the mixtures as the critical point of the solvent is approached.

Direct separation of boron from Na- and Ca-rich matrices by sublimation for stable isotope measurement by MC-ICP-MS.

PubMed

Wang, Bo-Shian; You, Chen-Feng; Huang, Kuo-Fang; Wu, Shein-Fu; Aggarwal, Suresh Kumar; Chung, Chuan-Hsiung; Lin, Pei-Ying

2010-09-15

An improved technique for precise and accurate determination of boron isotopic composition in Na-rich natural waters (groundwater, seawater) and marine biogenic carbonates was developed. This study used a 'micro-sublimation' technique to separate B from natural sample matrices in place of the conventional ion-exchange extraction. By adjusting analyte to appropriate pH, quantitative recovery of boron can be achieved (>98%) and the B procedural blank is limited to <8 pg. An additional mass bias effect in MC-ICP-MS was observed which could not be improved via the standard-sample-standard bracketing or the 'pseudo internal' normalization by Li. Therefore a standard other than NBS SRM 951 was used to monitor plasma condition in order to maintain analytical accuracy. An isotope cross-calibration with results from TIMS shows that the space-charge mass bias on MC-ICP-MS can be successfully corrected using off-line mathematical manipulation. Several reference materials, including the seawater IAPSO and two groundwater standards IAEA-B-2 and IAEA-B-3, were used to validate this approach. We found that the delta(11)B of the reference coral JCp-1 was 24.22+/-0.28 per thousand, corresponding to seawater pH based on the coral delta(11)B-pH function. Copyright (c) 2010 Elsevier B.V. All rights reserved.

The plasma separation process as a pre-cursor for large scale radioisotope production

NASA Astrophysics Data System (ADS)

Stevenson, Nigel R.

2001-07-01

Radioisotope production generally employs either accelerators or reactors to convert stable (usually enriched) isotopes into the desired product species. Radioisotopes have applications in industry, environmental sciences, and most significantly in medicine. The production of many potentially useful radioisotopes is significantly hindered by the lack of availability or by the high cost of key enriched stable isotopes. To try and meet this demand, certain niche enrichment processes have been developed and commercialized. Calutrons, centrifuges, and laser separation processes are some of the devices and techniques being employed to produce large quantities of selective enriched stable isotopes. Nevertheless, the list of enriched stable isotopes in sufficient quantities remains rather limited and this continues to restrict the availability of many radioisotopes that otherwise could have a significant impact on society. The Plasma Separation Process is a newly available commercial technique for producing large quantities of a wide range of enriched isotopes and thereby holds promise of being able to open the door to producing new and exciting applications of radioisotopes in the future.

Separation processes using expulsion from dilute supercritical solutions

DOEpatents

Cochran, H.D. Jr.

1993-04-20

A process is described for separating isotopes as well as other mixtures by utilizing the behavior of dilute repulsive or weakly attractive elements of the mixtures as the critical point of the solvent is approached.

Existing and emerging technologies for measuring stable isotope labelled retinol in biological samples: isotope dilution analysis of body retinol stores.

PubMed

Preston, Tom

2014-01-01

This paper discusses some of the recent improvements in instrumentation used for stable isotope tracer measurements in the context of measuring retinol stores, in vivo. Tracer costs, together with concerns that larger tracer doses may perturb the parameter under study, demand that ever more sensitive mass spectrometric techniques are developed. GCMS is the most widely used technique. It has high sensitivity in terms of sample amount and uses high resolution GC, yet its ability to detect low isotope ratios is limited by background noise. LCMSMS may become more accessible for tracer studies. Its ability to measure low level stable isotope tracers may prove superior to GCMS, but it is isotope ratio MS (IRMS) that has been designed specifically for low level stable isotope analysis through accurate analysis of tracer:tracee ratios (the tracee being the unlabelled species). Compound-specific isotope analysis, where GC is interfaced to IRMS, is gaining popularity. Here, individual 13C-labelled compounds are separated by GC, combusted to CO2 and transferred on-line for ratiometric analysis by IRMS at the ppm level. However, commercially-available 13C-labelled retinol tracers are 2 - 4 times more expensive than deuterated tracers. For 2H-labelled compounds, GC-pyrolysis-IRMS has now become more generally available as an operating mode on the same IRMS instrument. Here, individual compounds are separated by GC and pyrolysed to H2 at high temperature for analysis by IRMS. It is predicted that GC-pyrolysis-IRMS will facilitate low level tracer procedures to measure body retinol stores, as has been accomplished in the case of fatty acids and amino acids. Sample size requirements for GC-P-IRMS may exceed those of GCMS, but this paper discusses sample preparation procedures and predicts improvements, particularly in the efficiency of sample introduction.

Highly tritiated water processing by isotopic exchange

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shu, W.M.; Willms, R.S.; Glugla, M.

2015-03-15

Highly tritiated water (HTW) is produced in fusion machines and one of the promising technologies to process it is isotopic exchange. 3 kinds of Pt-catalyzed zeolite (13X-APG, CBV-100-CY and HiSiv-1000) were tested as candidates for isotopic exchange of highly tritiated water (HTW), and CBV-100-CY (Na-Y type with a SiO{sub 2}/Al{sub 2}O{sub 3} ratio of ∼ 5.0) shows the best performance. Small-scale tritium testing indicates that this method is efficient for reaching an exchange factor (EF) of 100. Full-scale non-tritium testing implies that an EF of 300 can be achieved in 24 hours of operation if a temperature gradient is appliedmore » along the column. For the isotopic exchange, deuterium recycled from the Isotope Separation System (deuterium with 1% T and/or 200 ppm T) should be employed, and the tritiated water regenerated from the Pt-catalyzed zeolite bed after isotopic exchange should be transferred to Water Detritiation System (WDS) for further processing.« less

Solid-state Marx based two-switch voltage modulator for the On-Line Isotope Mass Separator accelerator at the European Organization for Nuclear Research

NASA Astrophysics Data System (ADS)

Redondo, L. M.; Silva, J. Fernando; Canacsinh, H.; Ferrão, N.; Mendes, C.; Soares, R.; Schipper, J.; Fowler, A.

2010-07-01

A new circuit topology is proposed to replace the actual pulse transformer and thyratron based resonant modulator that supplies the 60 kV target potential for the ion acceleration of the On-Line Isotope Mass Separator accelerator, the stability of which is critical for the mass resolution downstream separator, at the European Organization for Nuclear Research. The improved modulator uses two solid-state switches working together, each one based on the Marx generator concept, operating as series and parallel switches, reducing the stress on the series stacked semiconductors, and also as auxiliary pulse generator in order to fulfill the target requirements. Preliminary results of a 10 kV prototype, using 1200 V insulated gate bipolar transistors and capacitors in the solid-state Marx circuits, ten stages each, with an electrical equivalent circuit of the target, are presented, demonstrating both the improved voltage stability and pulse flexibility potential wanted for this new modulator.

Chapter 13 Petrogenesis of the Campanian Ignimbrite: implications for crystal-melt separation and open-system processes from major and trace elements and Th isotopic data

USGS Publications Warehouse

Bohrson, W.A.; Spera, F.J.; Fowler, S.J.; Belkin, H.E.; de Vivo, B.; Rolandi, G.

2006-01-01

The Campanian Ignimbrite is a large-volume trachytic to phonolitic ignimbrite that was deposited at ???39.3 ka and represents one of a number of highly explosive volcanic events that have occurred in the region near Naples, Italy. Thermodynamic modeling using the MELTS algorithm reveals that major element variations are dominated by crystal-liquid separation at 0.15 GPa. Initial dissolved H2O content in the parental melt is ???3 wt.% and the magmatic system fugacity of oxygen was buffered along QFM+1. Significantly, MELTS results also indicate that the liquid line of descent is marked by a large change in the proportion of melt (from 0.46 to 0.09) at ???884??C, which leads to a discontinuity in melt composition (i.e., a compositional gap) and different thermodynamic and transport properties of melt and magma across the gap. Crystallization of alkali feldspar and plagioclase dominates the phase assemblage at this pseudo-invariant point temperature of ???884??C. Evaluation of the variations in the trace elements Zr, Nb, Th, U, Rb, Sm, and Sr using a mass balance equation that accounts for changing bulk mineral-melt partition coefficients as crystallization occurs indicates that crystal-liquid separation and open-system processes were important. Th isotope data yield an apparent isochron that is ???20 kyr younger than the age of the deposit, and age-corrected Th isotope data indicate that the magma body was an open system at the time of eruption. Because open-system behavior can profoundly change isotopic and elemental characteristics of a magma body, these Th results illustrate that it is critical to understand the contribution that open-system processes make to magmatic systems prior to assigning relevance to age or timescale information derived from such systems. Fluid-magma interaction has been proposed as a mechanism to change isotopic and elemental characteristics of magma bodies, but an evaluation of the mass and thermal constraints on such a process suggests

Protein Stable Isotope Fingerprinting (P-SIF): A New Tool to Understand Natural Isotopic Heterogeneity of Mixed Microbial Ecosystems

NASA Astrophysics Data System (ADS)

Pearson, A.; Mohr, W.; Tang, T.; Sattin, S.; Bovee, R.

2014-12-01

Protein stable isotope fingerprinting (P-SIF) is a method to measure the carbon isotope ratios of whole proteins separated from complex mixtures, including cultures and environmental samples. The goal of P-SIF is to expose the links between identity and function in microbial ecosystems by (i) determining the ratios of 13C/12C (values of δ13C) for different taxonomic divisions, and (ii) using those values as clues to the metabolic pathways employed by the respective organisms, while (iii) not perturbing the system, i.e., not adding exogenous substrates or isotope labels. To accomplish this, we employ two-dimensional HPLC to resolve a sample containing ca. 5-10 mg of mixed proteins into 960-1440 fractions. Each fraction then is split in two aliquots: The first is digested with trypsin for peptide sequencing, while the second is measured in triplicate using an isotope-ratio mass spectrometer interfaced with a spooling wire microcombustion device. Data from pure cultures show that bacteria have a narrow distribution of protein δ13C values within individual taxa (±0.7-1.2‰, 1σ). This is moderately larger than the mean precision of the triplicate isotope measurements (±0.5‰, 1σ) and may reflect heterogeneous distribution of 13C among the amino acids. When cells from different species are mixed together prior to protein extraction and separation, the results can predict accurately (to within ±1σ) the δ13C values of the original taxa. The number of data points required for this endmember prediction is ≥20/taxon, yielding a theoretical resolution of ca. 10 taxonomic units/sample. Initial tests on environmental samples suggest the approach will be useful to determine the overall trophic breadth of mixed microbial ecosystems.

Protein-based stable isotope probing.

PubMed

Jehmlich, Nico; Schmidt, Frank; Taubert, Martin; Seifert, Jana; Bastida, Felipe; von Bergen, Martin; Richnow, Hans-Hermann; Vogt, Carsten

2010-12-01

We describe a stable isotope probing (SIP) technique that was developed to link microbe-specific metabolic function to phylogenetic information. Carbon ((13)C)- or nitrogen ((15)N)-labeled substrates (typically with >98% heavy label) were used in cultivation experiments and the heavy isotope incorporation into proteins (protein-SIP) on growth was determined. The amount of incorporation provides a measure for assimilation of a substrate, and the sequence information from peptide analysis obtained by mass spectrometry delivers phylogenetic information about the microorganisms responsible for the metabolism of the particular substrate. In this article, we provide guidelines for incubating microbial cultures with labeled substrates and a protocol for protein-SIP. The protocol guides readers through the proteomics pipeline, including protein extraction, gel-free and gel-based protein separation, the subsequent mass spectrometric analysis of peptides and the calculation of the incorporation of stable isotopes into peptides. Extraction of proteins and the mass fingerprint measurements of unlabeled and labeled fractions can be performed in 2-3 d.

Understanding Copper Isotope Behavior in the High Temperature Magmatic-Hydrothermal Porphyry Environment

NASA Astrophysics Data System (ADS)

Gregory, Melissa J.; Mathur, Ryan

2017-11-01

Copper stable isotope geochemistry has the potential to constrain aspects of ore deposit formation once variations in the isotopic data can be related to the physiochemical conditions during metal deposition. This study presents Cu isotope ratios for samples from the Pebble porphyry Cu-Au-Mo deposit in Alaska. The δ65Cu values for hypogene copper sulfides range from -2.09‰ to 1.11‰ and show linear correlations with the δ18O isotope ratios calculated for the fluid in equilibrium with the hydrothermal alteration minerals in each sample. Samples with sodic-potassic, potassic, and illite alteration display a negative linear correlation between the Cu and O isotope results. This suggests that fractionation of Cu isotopes between the fluid and precipitating chalcopyrite is positive as the hydrothermal fluid is evolving from magmatic to mixed magmatic-meteoric compositions. Samples with advanced argillic alteration display a weak positive linear correlation between Cu and O isotope results consistent with small negative fluid-chalcopyrite Cu isotope fractionation during fluid evolution. The hydrothermal fluids that formed sodic-potassic, potassic, and illite alteration likely transported Cu as CuHS0. Hydrothermal fluids that resulted in advanced argillic alteration likely transport Cu as CuCl2-. The pH conditions also control Cu isotope fractionation, consistent with previous experimental work. Larger fractionation factors were found between fluids and chalcopyrite precipitating under neutral conditions contrasting with small fractionation factors calculated between fluids and chalcopyrite precipitating under acidic conditions. Therefore, this study proposes that hydrothermal fluid compositions and pH conditions are related to Cu isotope variations in high temperature magmatic-hydrothermal deposits.

High Precision Low-blank Lithium Isotope Ratios in Forams.

NASA Astrophysics Data System (ADS)

Misra, S.; Froelich, P. N.

2007-12-01

We present a high precision (±1‰, 2σ) low blank (<500 fg/ml) method for Li isotope measurements of forams using <2 ng of Li by single collector Quad ICP-MS (Agilent 7500cs). The Li isotope ratio of seawater (δ7Li) recorded in planktonic forams has the potential to constrain the evolution of seawater chemistry and elucidate the factors driving variations of oceanic mass balances linked to the continental and sea floor/hydrothermal silica cycles. In addition a δ7Li record of seawater will complement other long-term recorders of seawater chemistry such as Sr, Os and S isotopes. Li isotope measurements of forams are limited by several factors: low Li concentrations in forams (1-2 ppm), instrument-induced fractionation and mass bias effects, matrix effects, high Li blanks and incomplete recovery of Li during column separation. Modest concentrations of alkali and alkaline earth elements in the matrix result in variable mass bias in measured Li isotope ratios. Even worse, Li strongly fractionates during chromatographic clean-up to remove Na+, Ca2+ and Mg2+, from +100‰ in the leading edge to - 100‰ in the trailing edge of elution peaks (Urey 1938). Consequently, miniscule incomplete recoveries of Li during chromatographic separations can result in large unrecognized isotope fractionation of eluents. Large mass-dependent fractionation caused by a difference of 17% in mass between 6Li and 7Li, makes Li a powerful tracer of geochemical processes, but also promotes large and difficult-to-fix isotope fractionations during laboratory chemical processing. Matrix effects of Na & Ca and of column chromatography on Li isotope ratios were investigated using artificial Li solutions representative of foram compositions (matrix matching). Li/Ca and Li/Na ratios in cleaned forams are 10 μmol/mol and 3 mmol/mol respectively. An ICP-MS tolerance limit of 20 ppb for Na and 20 μM for Ca was established, much higher tolerances than by TIMS. A single step chromatographic method to

Extreme isotopic variations in the upper mantle: evidence from Ronda

NASA Astrophysics Data System (ADS)

Reisberg, Laurie; Zindler, Alan

1986-12-01

The Ronda Ultramafic Complex in southern Spain represents a piece of the Earth's mantle which has been tectonically emplaced into the crust. Nd and Sr isotopic analyses are presented for leached, hand-picked Cr-diopside separates prepared from 15 rock and 18 river sediment samples from Ronda. These results demonstrate that within this small, contiguous body there exists the entire range of Nd isotopic compositions, and much of the range of Sr compositions, found in rocks derived from the sub-oceanic mantle. The sediment cpx samples show that the average isotopic composition of the massif becomes progressively less "depleted" moving from SW to NE along the long axis of the massif. The rock cpx samples document 143Nd/ 144Nd variations from 0.5129 to 0.5126 and 87Sr/ 86Sr variations from 0.7031 to 0.7039 within a uniform outcrop less than 10 m in extent. Thus, extreme isotopic fluctuations exist over a wide range of wavelengths. Sr and Nd isotopes are generally inversely correlated, forming a trend on a Nd-Sr diagram that sharply crosscuts that of the "mantle array". Many of the 143Nd/ 144Nd values, and all of the Sm/Nd values, from one section of the massif are lower than that SCV015SCV0 of the bulk earth, implying that this region existed, or was influenced by a component which existed, in a LREE-enriched environment for a significant period of time. Among the sediment cpxs there is a positive correlation between 143Nd/ 144Nd and 147Sm/ 144Nd. The rock cpx separates display considerably more scatter. A simple, single-stage differentiation event starting with a uniform mantle source cannot explain these results. At least one episode of mixing with a LREE-enriched component is required. If these results from Ronda are typical of the upper mantle, basalts with different isotopic compositions need not derive from spatially separated mantle sources.

Microscopic model for the isotope effect in the high-Tc oxides

NASA Astrophysics Data System (ADS)

Kresin, V. Z.; Wolf, S. A.

1994-02-01

An unconventional microscopic mechanism relating Tc and the isotope substitution for the doped superconductors such as the high-Tc oxides is proposed. Strong nonadiabaticity, when it is impossible, strictly speaking, to separate fully the nuclear and electronic degrees of freedom, leads to a peculiar dependence of the carrier concentration n on the ionic mass M. This case corresponds, for example, to the isotopic substitution of the axial oxygen in YBa2Cu3O7-x. Because of the dependence of Tc on n, this leads to the dependence of Tc on M, that is to the isotope effect. The minimum value of the isotope coefficient corresponds to Tc=Tmaxc.

Isotope ratio mass spectrometry coupled to liquid and gas chromatography for wine ethanol characterization.

PubMed

Cabañero, Ana I; Recio, Jose L; Rupérez, Mercedes

2008-10-01

Two new procedures for wine ethanol 13C/12C isotope ratio determination, using high-performance liquid chromatography and gas chromatography isotope ratio mass spectrometry (HPLC/IRMS and GC/IRMS), have been developed to improve isotopic methods dedicated to the study of wine authenticity. Parameters influencing separation of ethanol from wine matrix such as column, temperature, mobile phase, flow rates and injection mode were investigated. Twenty-three wine samples from various origins were analyzed for validation of the procedures. The analytical precision was better than 0.15 per thousand, and no significant isotopic fractionation was observed employing both separative techniques coupled to IRMS. No significant differences and a very strong correlation (r = 0.99) were observed between the 13C/12C ratios obtained by the official method (elemental analyzer/isotope ratio mass spectrometry) and the proposed new methodology. The potential advantages of the developed methods over the traditional one are speed (reducing time required from hours to minutes) and simplicity. In addition, these are the first isotopic methods that allow 13C/12C determination directly from a liquid sample with no previous ethanol isolation, overcoming technical difficulties associated with sample treatment.

Protein Stable Isotope Fingerprinting (P-SIF): Multidimensional Protein Chromatography Coupled to Stable Isotope-Ratio Mass Spectrometry

NASA Astrophysics Data System (ADS)

Pearson, A.; Bovee, R. J.; Mohr, W.; Tang, T.

2012-12-01

As metagenomics increases our insight into microbial community diversity and metabolic potential, new approaches are required to determine the biogeochemical expression of this potential within ecosystems. Because stable isotopic analysis of the major bioactive elements (C, N) has been used historically to map flows of substrates and energy among macroscopic food webs, similar principles may apply to microbes. To address this challenge, we have developed a new analytical approach called Protein Stable Isotope Fingerprinting (P-SIF). P-SIF generates natural stable isotopic fingerprints of microbial individual or community proteomes. The main advantage of P-SIF is the potential to bridge the gap between diversity and function, thereby providing a window into the "black box" of environmental microbiology and helping to decipher the roles of uncultivated species. Our method implements a three-way, orthogonal scheme to separate mixtures of whole proteins into subfractions dominated by single or closely-related proteins. Protein extracts first are isoelectrically focused in a gel-free technique that yields 12 fractions separated over a gradient of pH 3-10. Each fraction then is separated by size-exclusion chromatography into 20 pools, ranging from >100kD to ~10kD. Finally, each of these pools is subjected to HPLC and collected in 40 time-slices based on protein hydrophobicity. Theoretical calculation reveals that the true chromatographic resolution of the total scheme is 5000, somewhat less than the 9600 resulting fractions. High-yielding fractions are subjected to δ13C analysis by spooling-wire microcombustion irMS (SWiM-irMS) optimized for samples containing 1-5 nmol carbon. Here we will present the method, results for a variety of pure cultures, and preliminary data for a sample of mixed environmental proteins. The data show the promise of this method for unraveling the metabolic complexity hidden within microbial communities.

Assessing compartmentalized flux in lipid metabolism with isotopes

DOE PAGES

Allen, Doug K.

2016-03-18

Metabolism in plants takes place across multiple cell types and within distinct organelles. The distributions equate to spatial heterogeneity; though the limited means to experimentally assess metabolism frequently involve homogenizing tissues and mixing metabolites from different locations.Most current isotope investigations of metabolism therefore lack the ability to resolve spatially distinct events. Recognition of this limitation has resulted in inspired efforts to advance metabolic flux analysis and isotopic labeling techniques. Though a number of these efforts have been applied to studies in central metabolism; recent advances in instrumentation and techniques present an untapped opportunity to make similar progress in lipid metabolismmore » where the use of stable isotopes has been more limited. These efforts will benefit from sophisticated radiolabeling reports that continue to enrich our knowledge on lipid biosynthetic pathways and provide some direction for stable isotope experimental design and extension of MFA. Evidence for this assertion is presented through the review of several elegant stable isotope studies and by taking stock of what has been learned from radioisotope investigations when spatial aspects of metabolism were considered. The studies emphasize that glycerolipid production occurs across several locations with assembly of lipids in the ER or plastid, fatty acid biosynthesis occurring in the plastid, and the generation of acetyl-CoA and glycerol-3-phosphate taking place at multiple sites. Considering metabolism in this context underscores the cellular and subcellular organization that is important to enhanced production of glycerolipids in plants. An attempt is made to unify salient features from a number of reports into a diagrammatic model of lipid metabolism and propose where stable isotope labeling experiments and further flux analysis may help address questions in the field.« less

Assessing compartmentalized flux in lipid metabolism with isotopes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Allen, Doug K.

Metabolism in plants takes place across multiple cell types and within distinct organelles. The distributions equate to spatial heterogeneity; though the limited means to experimentally assess metabolism frequently involve homogenizing tissues and mixing metabolites from different locations.Most current isotope investigations of metabolism therefore lack the ability to resolve spatially distinct events. Recognition of this limitation has resulted in inspired efforts to advance metabolic flux analysis and isotopic labeling techniques. Though a number of these efforts have been applied to studies in central metabolism; recent advances in instrumentation and techniques present an untapped opportunity to make similar progress in lipid metabolismmore » where the use of stable isotopes has been more limited. These efforts will benefit from sophisticated radiolabeling reports that continue to enrich our knowledge on lipid biosynthetic pathways and provide some direction for stable isotope experimental design and extension of MFA. Evidence for this assertion is presented through the review of several elegant stable isotope studies and by taking stock of what has been learned from radioisotope investigations when spatial aspects of metabolism were considered. The studies emphasize that glycerolipid production occurs across several locations with assembly of lipids in the ER or plastid, fatty acid biosynthesis occurring in the plastid, and the generation of acetyl-CoA and glycerol-3-phosphate taking place at multiple sites. Considering metabolism in this context underscores the cellular and subcellular organization that is important to enhanced production of glycerolipids in plants. An attempt is made to unify salient features from a number of reports into a diagrammatic model of lipid metabolism and propose where stable isotope labeling experiments and further flux analysis may help address questions in the field.« less

Compound-specific isotope analysis: Questioning the origins of a trichloroethene plume

USGS Publications Warehouse

Eberts, S.M.; Braun, C.; Jones, S.

2008-01-01

Stable carbon isotope ratios of trichloroethene (TCE), cis-1,2- dichloroethene, and trans-1,2-dichloroethene were determined by use of gas chromatography-combustion-isotope ratio mass spectroscopy to determine whether compound-specific stable carbon isotopes could be used to help understand the origin and history of a TCE groundwater plume in Fort Worth, TX. Calculated ??13C values for total chlorinated ethenes in groundwater samples, which can approximate the ??13C of a spilled solvent if all degradation products are accounted for, were useful for determining whether separate lobes of the plume resulted from different sources. Most notably, values for one lobe, where tetrachloroethene (PCE) has been detected periodically, were outside the range for manufactured TCE but within the range for manufactured PCE, whereas values for a separate lobe, which is downgradient of reported TCE spills, were within the range for manufactured TCE. Copyright ?? Taylor & Francis Group, LLC.

Precise Analysis of Gallium Isotopic Composition by MC-ICP-MS.

PubMed

Yuan, Wei; Chen, Jiu Bin; Birck, Jean-Louis; Yin, Zuo Ying; Yuan, Sheng Liu; Cai, Hong Ming; Wang, Zhong Wei; Huang, Qiang; Wang, Zhu Hong

2016-10-04

Though an isotope approach could be beneficial for better understanding the biogeochemical cycle of gallium (Ga), an analogue of the monoisotopic element aluminum (Al), the geochemistry of Ga isotopes has not been widely elaborated. We developed a two-step method for purifying Ga from geological (biological) samples for precise measurement of Ga isotope ratio using multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS). Ga was thoroughly separated from other matrix elements using two chromatographic columns loaded with AG 1-X4 and Ln-spec resin, respectively. The separation method was carefully calibrated using both synthetic and natural samples and validated by assessing the extraction yield (99.8 ± 0.8%, 2SD, n = 23) and the reproducibility (2SD uncertainty better than 0.05‰, n = 116) of the measured isotopic ratio (expressed as δ 71 Ga). The validation of the whole protocol, together with instrumental analysis, was confirmed by the investigation of the matrix effect, the result of a standard addition experiment, and the comparison of Ga isotope measurement on two mass spectrometers-Nu Plasma II and Neptune Plus. Although the measurements using the sample-standard bracketing (SSB) correction method on both instruments resulted in identical δ 71 Ga values for reference materials, the modified empirical external normalization (MEEN) method gave relatively better precision compared to SSB on Neptune. Our preliminary results showed large variation of δ 71 Ga (up to 1.83‰) for 10 standards, with higher values in industrially produced materials, implying potential application of Ga isotopes.

Oxygen isotope geochemistry of the amphiboles: isotope effects of cation substitutions in minerals

NASA Astrophysics Data System (ADS)

Kohn, Matthew J.; Valley, John W.

1998-06-01

The occurrence of coexisting amphiboles in rocks and the likelihood of concurrent isotope closure allows equilibrium oxygen isotope fractionations among the amphiboles to be recovered from natural samples. Oxygen isotope analyses of mineral separates using laser fluorination show that coexisting amphiboles increasingly partition 18O in the order: hornblende ≪ gedrite < cummingtonite ≤ anthophyllite. The observed fractionations at ˜575°C are: Δ(Ged-Hbl) = 0.8‰, Δ(Cum-Hbl) = 0.9, Δ(Cum-Ged) = 0.2, Δ(Ath-Ged) = 0.3, and Δ(Ath-Hbl) > 0.9. Previously published data for hornblende, actinolite, glaucophane, and garnet show that Δ(Act-Hbl) ˜ 0.2, Δ(Gln-Grt) ≫ 1, and Δ(Hbl-Grt) ˜ 0. Thus, glaucophane strongly partitions 18O relative to the calcic amphiboles. The fractionation between two amphiboles of arbitrary composition can be predicted from the known fractionations for mica endmembers, pyroxene endmembers, and exchange components such as CaAl(NaSi) -1, NaAl(CaMg) -1, CaMg -1, MgFe -1, FeMn -1, KNa -1, KAl( Si) -1, and Fe 3+Al -1. Applications of the exchange component method reproduce measured amphibole fractionations to within ±0.1 to ±0.2‰, whereas other predictive methods cause misfit for typical metamorphic hornblende of ≥0.5‰ at 575°C. Although the isotope effects of cation exchanges may be small at high-T, they magnify dramatically for minerals formed in surficial, diagenetic, and low-T metamorphic environments. Different composition clays are predicted to have equilibrium δ 18O differences of 2-9‰. If the isotope fractionation can be determined for one mineral endmember, then calibrated exchanges allow accurate prediction of the isotope fractionations for intermediate compositions of most ortho-, ring-, chain-, and sheet-silicates.

Multi-purpose hydrogen isotopes separation plant design

DOE Office of Scientific and Technical Information (OSTI.GOV)

Boniface, H.A.; Gnanapragasam, N.V.; Ryland, D.K.

2015-03-15

There is a potential interest at AECL's Chalk River Laboratories to remove tritium from moderately tritiated light water and to reclaim tritiated, downgraded heavy water. With only a few limitations, a single CECE (Combined Electrolysis and Catalytic Exchange) process configuration can be designed to remove tritium from heavy water or light water and upgrade heavy water. Such a design would have some restrictions on the nature of the feed-stock and tritium product, but could produce essentially tritium-free light or heavy water that is chemically pure. The extracted tritium is produced as a small quantity of tritiated heavy water. The overallmore » plant capacity is fixed by the total amount of electrolysis and volume of catalyst. In this proposal, with 60 kA of electrolysis a throughput of 15 kg*h{sup -1} light water for detritiation, about 4 kg*h{sup -1} of heavy water for detritiation and about 27 kg*h{sup -1} of 98% heavy water for upgrading can be processed. Such a plant requires about 1,000 liters of AECL isotope exchange catalyst. The general design features and details of this multi-purpose CECE process are described in this paper, based on some practical choices of design criteria. In addition, we outline the small differences that must be accommodated and some compromises that must be made to make the plant capable of such flexible operation. (authors)« less

Empirical calibration of the clinopyroxene-garnet magnesium isotope geothermometer and implications

NASA Astrophysics Data System (ADS)

Li, Wang-Ye; Teng, Fang-Zhen; Xiao, Yilin; Gu, Hai-Ou; Zha, Xiang-Ping; Huang, Jian

2016-07-01

The large equilibrium Mg isotope fractionation between clinopyroxene and garnet observed in eclogites makes it a potential high-precision geothermometer, but calibration of this thermometer by natural samples is still limited. Here, we report Mg isotopic compositions of eclogite whole rocks as well as Mg and O isotopic compositions of clinopyroxene and garnet separates from 16 eclogites that formed at different temperatures from the Dabie orogen, China. The whole-rock δ26Mg values vary from -1.20 to +0.10 ‰. Among them, 11 samples display limited δ26Mg variations from -0.36 to -0.17 ‰, similar to those of their protoliths. The mineral separates exhibit very different δ26Mg values, from -0.39 to +0.39 ‰ for clinopyroxenes and from -1.94 to -0.81 ‰ for garnets. The clinopyroxene-garnet Mg isotope fractionation (Δ26Mgclinopyroxene-garnet = δ26Mgclinopyroxene-δ26Mggarnet) varies from 1.05 to 2.15 ‰. The clinopyroxene-garnet O isotope fractionation (Δ18Oclinopyroxene-garnet = δ18Oclinopyroxene-δ18Ogarnet) varies from -1.01 to +0.98 ‰. Equilibrium Mg isotope fractionation between clinopyroxene and garnet in the investigated samples is selected based on both the δ26Mgclinopyroxene versus δ26Mggarnet plot and the state of O isotope equilibrium between clinopyroxene and garnet. The equilibrium Δ26Mgclinopyroxene-garnet and corresponding temperature data obtained in this study, together with those available so far in literatures for natural eclogites, are used to calibrate the clinopyroxene-garnet Mg isotope thermometer. This yields a function of Δ26Mgclinopyroxene-garnet = (0.99 ± 0.06) × 106/ T 2, where T is temperature in Kelvin. The refined function not only provides the best empirically calibrated clinopyroxene-garnet Mg isotope thermometer for precise constraints of temperatures of clinopyroxene- and garnet-bearing rocks, but also has potential applications in high-temperature Mg isotope geochemistry.

Chlorine isotope effects from isotope ratio mass spectrometry suggest intramolecular C-Cl bond competition in trichloroethene (TCE) reductive dehalogenation.

PubMed

Cretnik, Stefan; Bernstein, Anat; Shouakar-Stash, Orfan; Löffler, Frank; Elsner, Martin

2014-05-20

Chlorinated ethenes are prevalent groundwater contaminants. To better constrain (bio)chemical reaction mechanisms of reductive dechlorination, the position-specificity of reductive trichloroethene (TCE) dehalogenation was investigated. Selective biotransformation reactions (i) of tetrachloroethene (PCE) to TCE in cultures of Desulfitobacterium sp. strain Viet1; and (ii) of TCE to cis-1,2-dichloroethene (cis-DCE) in cultures of Geobacter lovleyi strain SZ were investigated. Compound-average carbon isotope effects were -19.0‰ ± 0.9‰ (PCE) and -12.2‰ ± 1.0‰ (TCE) (95% confidence intervals). Using instrumental advances in chlorine isotope analysis by continuous flow isotope ratio mass spectrometry, compound-average chorine isotope effects were measured for PCE (-5.0‰ ± 0.1‰) and TCE (-3.6‰ ± 0.2‰). In addition, position-specific kinetic chlorine isotope effects were determined from fits of reactant and product isotope ratios. In PCE biodegradation, primary chlorine isotope effects were substantially larger (by -16.3‰ ± 1.4‰ (standard error)) than secondary. In TCE biodegradation, in contrast, the product cis-DCE reflected an average isotope effect of -2.4‰ ± 0.3‰ and the product chloride an isotope effect of -6.5‰ ± 2.5‰, in the original positions of TCE from which the products were formed (95% confidence intervals). A greater difference would be expected for a position-specific reaction (chloride would exclusively reflect a primary isotope effect). These results therefore suggest that both vicinal chlorine substituents of TCE were reactive (intramolecular competition). This finding puts new constraints on mechanistic scenarios and favours either nucleophilic addition by Co(I) or single electron transfer as reductive dehalogenation mechanisms.

Advanced inorganic separators for alkaline batteries

NASA Technical Reports Server (NTRS)

Sheibley, D. W. (Inventor)

1982-01-01

A flexible, porous battery separator comprising a coating applied to a porous, flexible substrate is described. The coating comprises: (1) a thermoplastic rubber-based resin which is insoluble and unreactive in the alkaline electrolyte; (2) a polar organic plasticizer which is reactive with the alkaline electrolyte to produce a reaction product which contains a hydroxyl group and/or a carboxylic acid group; and (3) a mixture of polar particulate filler materials which are unreactive with the electrolyte, the mixture comprising at least one first filler material having a surface area of greater than 25 meters sq/gram, at least one second filler material having a surface area of 10 to 25 sq meters/gram, wherein the volume of the mixture of filler materials is less than 45% of the total volume of the fillers and the binder, the filler surface area per gram of binder is about 20 to 60 sq meters/gram, and the amount of plasticizer is sufficient to coat each filler particle. A method of forming the battery separator is also described.

Simultaneous stable carbon isotopic analysis of wine glycerol and ethanol by liquid chromatography coupled to isotope ratio mass spectrometry.

PubMed

Cabañero, Ana I; Recio, Jose L; Rupérez, Mercedes

2010-01-27

A novel procedure was established for the simultaneous characterization of wine glycerol and ethanol (13)C/(12)C isotope ratio, using liquid chromatography/isotope ratio mass spectrometry (LC-IRMS). Several parameters influencing separation of glycerol and ethanol from wine matrix were optimized. Results obtained for 35 Spanish samples exposed no significant differences and very strong correlations (r = 0.99) between the glycerol (13)C/(12)C ratios obtained by an alternative method (gas chromatography/isotope ratio mass spectrometry) and the proposed new methodology, and between the ethanol (13)C/(12)C ratios obtained by the official method (elemental analyzer/isotope ratio mass spectrometry) and the proposed new methodology. The accuracy of the proposed method varied from 0.01 to 0.19 per thousand, and the analytical precision was better than 0.25 per thousand. The new developed LC-IRMS method it is the first isotopic method that allows (13)C/(12)C determination of both analytes in the same run directly from a liquid sample with no previous glycerol or ethanol isolation, overcoming technical difficulties associated with complex sample treatment and improving in terms of simplicity and speed.

Theoretical description of quantum mechanical permeation of graphene membranes by charged hydrogen isotopes

NASA Astrophysics Data System (ADS)

Mazzuca, James W.; Haut, Nathaniel K.

2018-06-01

It has been recently shown that in the presence of an applied voltage, hydrogen and deuterium nuclei can be separated from one another using graphene membranes as a nuclear sieve, resulting in a 10-fold enhancement in the concentration of the lighter isotope. While previous studies, both experimental and theoretical, have attributed this effect mostly to differences in vibrational zero point energy (ZPE) of the various isotopes near the membrane surface, we propose that multi-dimensional quantum mechanical tunneling of nuclei through the graphene membrane influences this proton permeation process in a fundamental way. We perform ring polymer molecular dynamics calculations in which we include both ZPE and tunneling effects of various hydrogen isotopes as they permeate the graphene membrane and compute rate constants across a range of temperatures near 300 K. While capturing the experimentally observed separation factor, our calculations indicate that the transverse motion of the various isotopes across the surface of the graphene membrane is an essential part of this sieving mechanism. An understanding of the multi-dimensional quantum mechanical nature of this process could serve to guide the design of other such isotopic enrichment processes for a variety of atomic and molecular species of interest.

Theoretical description of quantum mechanical permeation of graphene membranes by charged hydrogen isotopes.

PubMed

Mazzuca, James W; Haut, Nathaniel K

2018-06-14

It has been recently shown that in the presence of an applied voltage, hydrogen and deuterium nuclei can be separated from one another using graphene membranes as a nuclear sieve, resulting in a 10-fold enhancement in the concentration of the lighter isotope. While previous studies, both experimental and theoretical, have attributed this effect mostly to differences in vibrational zero point energy (ZPE) of the various isotopes near the membrane surface, we propose that multi-dimensional quantum mechanical tunneling of nuclei through the graphene membrane influences this proton permeation process in a fundamental way. We perform ring polymer molecular dynamics calculations in which we include both ZPE and tunneling effects of various hydrogen isotopes as they permeate the graphene membrane and compute rate constants across a range of temperatures near 300 K. While capturing the experimentally observed separation factor, our calculations indicate that the transverse motion of the various isotopes across the surface of the graphene membrane is an essential part of this sieving mechanism. An understanding of the multi-dimensional quantum mechanical nature of this process could serve to guide the design of other such isotopic enrichment processes for a variety of atomic and molecular species of interest.

Advances in covalent organic frameworks in separation science.

PubMed

Qian, Hai-Long; Yang, Cheng-Xiong; Wang, Wen-Long; Yang, Cheng; Yan, Xiu-Ping

2018-03-23

Covalent organic frameworks (COFs) are a new class of multifunctional crystalline organic polymer constructed with organic monomers via robust covalent bonds. The unique properties such as convenient modification, low densities, large specific surface areas, good stability and permanent porosity make COFs great potential in separation science. This review shows the state-of-the art for the application of COFs and their composites in analytical separation science. COFs and their composites have been explored as promising sorbents for solid phase extraction, potential coatings for solid phase microextraction, and novel stationary phases for gas chromatography, high-performance liquid chromatography and capillary electrochromatography. The prospects of COFs for separation science are also presented, which can offer an outlook and reference for further study on the applications of COFs. Copyright © 2018 Elsevier B.V. All rights reserved.

Nickel isotopic composition of the mantle

NASA Astrophysics Data System (ADS)

Gall, Louise; Williams, Helen M.; Halliday, Alex N.; Kerr, Andrew C.

2017-02-01

This paper presents a detailed high-precision study of Ni isotope variations in mantle peridotites and their minerals, komatiites as well as chondritic and iron meteorites. Ultramafic rocks display a relatively large range in δ60 Ni (permil deviation in 60 Ni /58 Ni relative to the NIST SRM 986 Ni isotope standard) for this environment, from 0.15 ± 0.07‰ to 0.36 ± 0.08‰, with olivine-rich rocks such as dunite and olivine cumulates showing lighter isotope compositions than komatiite, lherzolite and pyroxenite samples. The data for the mineral separates shed light on the origin of these variations. Olivine and orthopyroxene display light δ60 Ni whereas clinopyroxene and garnet are isotopically heavy. This indicates that peridotite whole-rock δ60 Ni may be controlled by variations in modal mineralogy, with the prediction that mantle melts will display variable δ60 Ni values due to variations in residual mantle and cumulate mineralogy. Based on fertile peridotite xenoliths and Phanerozoic komatiite samples it is concluded that the upper mantle has a relatively homogeneous Ni isotope composition, with the best estimate of δ60Nimantle being 0.23 ± 0.06‰ (2 s.d.). Given that >99% of the Ni in the silicate Earth is located in the mantle, this also defines the Ni isotope composition of the Bulk Silicate Earth (BSE). This value is nearly identical to the results obtained for a suite of chondrites and iron meteorites (mean δ60 Ni 0.26 ± 0.12‰ and 0.29 ± 0.10‰, respectively) showing that the BSE is chondritic with respect to its Ni isotope composition, with little to no Ni mass-dependent isotope fractionation resulting from core formation.

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS

NASA Technical Reports Server (NTRS)

Socki, Richard A.; Fu, Qi; Niles, Paul B.

2011-01-01

One possible process responsible for methane generation on Mars is abiotic formation by Fischer-Tropsch-type (FTT) synthesis during serpentinization reactions. Measurement of carbon and hydrogen isotopes of intermediary organic compounds can help constrain the origin of this methane by tracing the geochemical pathway during formation. Of particular interest within the context of this work is the isotopic composition of organic intermediaries produced on the surfaces of mineral catalysts (i.e. magnetite) during hydrothermal experiments, and the ability to make meaningful and reproducible hydrogen isotope measurements. Reported here are results of experiments to characterize the hydrogen isotope composition of low molecular weight organic acids and alcohols. The presence of these organic compounds has been suggested by others as intermeadiary products made during mineral surface catalyzed reactions. This work compliments our previous study characterizing the carbon isotope composition of similar low molecular weight intermediary organic compounds (Socki, et al, American Geophysical Union Fall meeting, Abstr. #V51B-2189, Dec., 2010). Our hydrogen isotope measurements utilize a unique analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). Our technique is unique in that it carries a split of the pyrolyzed GC-separated product to a Thermo DSQ-II? quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Iron Isotopes in Meteorites

NASA Astrophysics Data System (ADS)

Kehm, K.; Alexander, C. M.; Hauri, E. H.

2001-12-01

The recent identification of naturally occurring isotopic mass fractionation of the transition met-als on the Earth has prompted a search for similar variability in meteorites. Studies of Cu, Zn, and Fe, for example, have revealed per-mil level and larger mass fractionations between different bulk meteorites. Such variations can result from temperature-sensitive isotope exchange reactions and kinetic processes, and therefore may reflect conditions in the solar nebula and on meteorite parent bodies. Recent advances in ICP-MS have permitted isotope studies of transition metals and other elements with similarly small isotopic mass dispersions. Among the transition metals, Fe is perhaps the most difficult to analyze by ICP-MS because plasma sources are copious producers of argide molecules that interfere with the measurement of iron isotopes. However, the stable isotope behavior of Fe is of special interest because it is a non-refractory major element in meteorites, present in a variety of mineral associations and redox states. Considerable effort has gone into overcoming the inherent analytical difficulties of measuring Fe using ICP-MS. We recently reported on a technique that achieves argide reduction by operating the plasma source in so-called 'cold' mode. In this presentation, we report results from this ongoing work. To date, analyses of nine different meteorites, and eight individual Tieschitz (H3) chondrules have been completed, along with a number of measurements of the Hawaiian basalt sample Kil1919. All of the bulk meteorite compositions, which include both chondrites and irons, have identical 56Fe/54Fe to within ~ 0.14 per mil (2 sigma), and are indistinguishable from the composition of the terrestrial basalt. The Tieschitz chondrules, on the other hand, tend to have isotopically light compositions. This could reflect formation from fractionated starting material. Alternatively, Fe condensation, under non-equilibrium conditions can enrich light isotopes

High Resolution Gamma Ray Analysis of Medical Isotopes

NASA Astrophysics Data System (ADS)

Chillery, Thomas

2015-10-01

Compton-suppressed high-purity Germanium detectors at the University of Massachusetts Lowell have been used to study medical radioisotopes produced at Brookhaven Linac Isotope Producer (BLIP), in particular isotopes such as Pt-191 used for cancer therapy in patients. The ability to precisely analyze the concentrations of such radio-isotopes is essential for both production facilities such as Brookhaven and consumer hospitals across the U.S. Without accurate knowledge of the quantities and strengths of these isotopes, it is possible for doctors to administer incorrect dosages to patients, thus leading to undesired results. Samples have been produced at Brookhaven and shipped to UML, and the advanced electronics and data acquisition capabilities at UML have been used to extract peak areas in the gamma decay spectra. Levels of Pt isotopes in diluted samples have been quantified, and reaction cross-sections deduced from the irradiation parameters. These provide both cross checks with published work, as well as a rigorous quantitative framework with high quality state-of-the-art detection apparatus in use in the experimental nuclear physics community.

The South African isotope facility project

NASA Astrophysics Data System (ADS)

Bark, R. A.; Barnard, A. H.; Conradie, J. L.; de Villiers, J. G.; van Schalkwyk, P. A.

2018-05-01

The South African Isotope Facility (SAIF) is a project in which iThemba LABS plans to build a radioactive-ion beam (RIB) facility. The project is divided into the Accelerator Centre of Exotic Isotopes (ACE Isotopes) and the Accelerator Centre for Exotic Beams (ACE Beams). For ACE Isotopes, a high-current, 70 MeV cyclotron will be acquired to take radionuclide production off the existing Separated Sector Cyclotron (SSC). A freed up SSC will then be available for an increased tempo of nuclear physics research and to serve as a driver accelerator for the ACE Beams project, in which protons will be used for the direct fission of Uranium, producing beams of fission fragments. The ACE Beams project has begun with "LeRIB" - a Low Energy RIB facility, now under construction. In a collaboration with INFN Legnaro, the target/ion-source "front-end" will be a copy of the front-end developed for the SPES project. A variety of targets may be inserted into the SPES front-end; a uranium-carbide target has been designed to produce up to 2 × 1013 fission/s using a 70 MeV proton beam of 150 µA intensity.

Long-term fertilization alters chemically-separated soil organic carbon pools: Based on stable C isotope analyses

NASA Astrophysics Data System (ADS)

Dou, Xiaolin; He, Ping; Cheng, Xiaoli; Zhou, Wei

2016-01-01

Quantification of dynamics of soil organic carbon (SOC) pools under the influence of long-term fertilization is essential for predicting carbon (C) sequestration. We combined soil chemical fractionation with stable C isotope analyses to investigate the C dynamics of the various SOC pools after 25 years of fertilization. Five types of soil samples (0-20, 20-40 cm) including the initial level (CK) and four fertilization treatments (inorganic nitrogen fertilizer, IN; balanced inorganic fertilizer, NPK; inorganic fertilizer plus farmyard manure, MNPK; inorganic fertilizer plus corn straw residue, SNPK) were separated into recalcitrant and labile fractions, and the fractions were analysed for C content, C:N ratios, δ13C values, soil C and N recalcitrance indexes (RIC and RIN). Chemical fractionation showed long-term MNPK fertilization strongly increased the SOC storage in both soil layers (0-20 cm = 1492.4 gC m2 and 20-40 cm = 1770.6 gC m2) because of enhanced recalcitrant C (RC) and labile C (LC). The 25 years of inorganic fertilizer treatment did not increase the SOC storage mainly because of the offsetting effects of enhanced RC and decreased LC, whereas no clear SOC increases under the SNPK fertilization resulted from the fast decay rates of soil C.

Long-term fertilization alters chemically-separated soil organic carbon pools: Based on stable C isotope analyses.

PubMed

Dou, Xiaolin; He, Ping; Cheng, Xiaoli; Zhou, Wei

2016-01-11

Quantification of dynamics of soil organic carbon (SOC) pools under the influence of long-term fertilization is essential for predicting carbon (C) sequestration. We combined soil chemical fractionation with stable C isotope analyses to investigate the C dynamics of the various SOC pools after 25 years of fertilization. Five types of soil samples (0-20, 20-40 cm) including the initial level (CK) and four fertilization treatments (inorganic nitrogen fertilizer, IN; balanced inorganic fertilizer, NPK; inorganic fertilizer plus farmyard manure, MNPK; inorganic fertilizer plus corn straw residue, SNPK) were separated into recalcitrant and labile fractions, and the fractions were analysed for C content, C:N ratios, δ(13)C values, soil C and N recalcitrance indexes (RIC and RIN). Chemical fractionation showed long-term MNPK fertilization strongly increased the SOC storage in both soil layers (0-20 cm = 1492.4 gC m(2) and 20-40 cm = 1770.6 gC m(2)) because of enhanced recalcitrant C (RC) and labile C (LC). The 25 years of inorganic fertilizer treatment did not increase the SOC storage mainly because of the offsetting effects of enhanced RC and decreased LC, whereas no clear SOC increases under the SNPK fertilization resulted from the fast decay rates of soil C.

Isotope ratio analysis of individual sub-micrometer plutonium particles with inductively coupled plasma mass spectrometry.

PubMed

Esaka, Fumitaka; Magara, Masaaki; Suzuki, Daisuke; Miyamoto, Yutaka; Lee, Chi-Gyu; Kimura, Takaumi

2010-12-15

Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles. Copyright © 2010 Elsevier B.V. All rights reserved.

Segregation of isotopes of heavy metals due to light-induced drift: results and problems

NASA Astrophysics Data System (ADS)

Sapar, A.; Aret, A.; Poolamäe, R.; Sapar, L.

2008-04-01

Atutov and Shalagin (1988) proposed light-induced drift (LID) as a physically well understandable mechanism to explain the formation of isotopic anomalies observed in CP stars. We have generalized the theory of LID and applied it to diffusion of heavy elements and their isotopes in quiescent atmospheres of CP stars. Diffusional segregation of isotopes of chemical elements is described by the equations of continuity and diffusion velocity. Computations of evolutionary sequences for the abundances of mercury isotopes in several model atmospheres have been made, using the Fortran 90 program SMART composed by the authors. Results confirm predominant role of LID in separation of isotopes.

Stable Isotope Systematics of Martian Perchlorate

NASA Astrophysics Data System (ADS)

Martin, P.; Farley, K. A.; Archer, D., Jr.; Atreya, S. K.; Conrad, P. G.; Eigenbrode, J. L.; Fairen, A.; Franz, H. B.; Freissinet, C.; Glavin, D. P.; Mahaffy, P. R.; Malespin, C.; Ming, D. W.; Navarro-Gonzalez, R.; Sutter, B.

2015-12-01

Chlorine isotopic compositions in HCl released during evolved gas analysis (EGA) runs have been detected by the Sample Analysis at Mars (SAM) instrument on the Curiosity rover ranging from approximately -9‰ to -50‰ δ37Cl, with two spatially and isotopically separated groups of samples averaging -15‰ and -45‰. These extremely low values are the first such detection of any known natural material; common terrestrial values very rarely exceed ±5‰, and the most extreme isotopic signature yet detected elsewhere in the solar system are values of around +24‰ on the Moon. The only other known location in the solar system with large negative chlorine isotopes is the Atacama Desert, where perchlorate with -14‰ δ37Cl has been detected. The Atacama perchlorate has unusual Δ17O signatures associated with it, indicating a formation mechanism involving O3, which suggests an atmospheric origin of the perchlorate and associated large isotopic anomalies. Identification of non-zero positive Δ17O signatures in the O2 released during EGA runs would allow definitive evidence for a similar process having occurred on Mars. Perchlorate is thought to be the most likely source of HCl in EGA runs due to the simultaneous onset of O2 release. If perchlorate is indeed the HCl source, atmospheric chemistry could be responsible for the observed isotopic anomalies, with variable extents of perchlorate production producing the isotopic variability. However, chloride salts have also been observed to release HCl upon heating; if the timing of O2 release is merely coincidental, observed HCl could be coming from chlorides. At thermodynamic equilibrium, the fractionation factor of perchlorate reduction is 0.93, meaning that differing amounts of post-deposition reduction of isotopically normal perchlorate to chloride could account for the highly variable Cl isotopes. Additionally, post-deposition reduction could account for the difference between the two Cl isotopic groups if perchlorate

Dual-isotope PET using positron-gamma emitters.

PubMed

Andreyev, A; Celler, A

2011-07-21

Positron emission tomography (PET) is widely recognized as a highly effective functional imaging modality. Unfortunately, standard PET cannot be used for dual-isotope imaging (which would allow for simultaneous investigation of two different biological processes), because positron-electron annihilation products from different tracers are indistinguishable in terms of energy. Methods that have been proposed for dual-isotope PET rely on differences in half-lives of the participating isotopes; these approaches, however, require making assumptions concerning kinetic behavior of the tracers and may not lead to optimal results. In this paper we propose a novel approach for dual-isotope PET and investigate its performance using GATE simulations. Our method requires one of the two radioactive isotopes to be a pure positron emitter and the second isotope to emit an additional high-energy gamma in a cascade simultaneously with positron emission. Detection of this auxiliary prompt gamma in coincidence with the annihilation event allows us to identify the corresponding 511 keV photon pair as originating from the same isotope. Two list-mode datasets are created: a primary dataset that contains all detected 511 keV photon pairs from both isotopes, and a second, tagged (much smaller) dataset that contains only those PET events for which a coincident prompt gamma has also been detected. An image reconstructed from the tagged dataset reflects the distribution of the second positron-gamma radiotracer and serves as a prior for the reconstruction of the primary dataset. Our preliminary simulation study with partially overlapping (18)F/(22)Na and (18)F/(60)Cu radiotracer distributions showed that in these two cases the dual-isotope PET method allowed for separation of the two activity distributions and recovered total activities with relative errors of about 5%.

Carbon isotopic analysis of atmospheric methane by isotope-ratio-monitoring gas chromatography-mass spectrometry

NASA Technical Reports Server (NTRS)

Merritt, Dawn A.; Hayes, J. M.; Des Marais, David J.

1995-01-01

Less than 15 min are required for the determination of delta C(sub PDB)-13 with a precision of 0.2 ppt(1 sigma, single measurement) in 5-mL samples of air containing CH4 at natural levels (1.7 ppm). An analytical system including a sample-introduction unit incorporating a preparative gas chromatograph (GC) column for separation of CH4 from N2, O2, and Ar is described. The 15-min procedure includes time for operation of that system, high-resolution chromatographic separation of the CH4, on-line combustion and purification of the products, and isotopic calibration. Analyses of standards demonstrate that systematic errors are absent and that there is no dependence of observed values of delta on sample size. For samples containing 100 ppm or more CH4, preconcentration is not required and the analysis time is less than 5 min. The system utilizes a commercially available, high-sensitivity isotope-ratio mass spectrometer. For optimal conditions of smaple handling and combustion, performance of the system is within a factor of 2 of the shot-noise limit. The potential exists therefore for analysis of samples as small as 15 pmol CH4 with a standard deviation of less than 1 ppt.

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

NASA Technical Reports Server (NTRS)

Boering, Kristie A.; Connell, Peter; Rotman, Douglas

2004-01-01

We investigated the isotopic fractionation of CH4 and hydrogen (H2) in the stratosphere by incorporating isotope-specific rate coefficients into the Lawrence Livermore National Laboratory (LLNL) 2D model and comparing the model results with new observations from the NASA ER-2 aircraft (funded through a separate task under the Upper Atmosphere Research Program). The model results reveal that fractionation which occurs in the stratosphere has a significant influence on isotope compositions in the free troposphere, an important point which had previously been ignored, unrecognized or unquantified for many long-lived trace gases, including CH4 and H2 which we have focused our efforts on to date. Our analyses of the model results and new isotope observations have also been used to test how well the kinetic isotope effects are known, at least to within the uncertainties in model chemistry and transport. Overall, these results represent an important step forward in our understanding of isotope fractionation in the atmosphere and demonstrate that stratospheric isotope fractionation cannot be ignored in modeling studies which use isotope observations in the troposphere to infer the global budgets of CH4 (an important greenhouse gas) and of H2 (a gas whose atmospheric budget must be better quantified, particularly before a large human perturbation from fuel cell use is realized). Our analyses of model results and observations from the NASA ER-2 aircraft are briefly summarized separately below for CH4, H2, and H2O and for the contribution of these modeling studies to date to our understanding of isotope fractionation for N2O, CO2, and O3 as well.

Small Stirling dynamic isotope power system for multihundred-watt robotic missions

NASA Technical Reports Server (NTRS)

Bents, David J.

1991-01-01

Free Piston Stirling Engine (FPSE) and linear alternator (LA) technology is combined with radioisotope heat sources to produce a compact dynamic isotope power system (DIPS) suitable for multihundred watt space application which appears competitive with advance radioisotope thermoelectric generators (RTGs). The small Stirling DIPS is scalable to multihundred watt power levels or lower. The FPSE/LA is a high efficiency convertor in sizes ranging from tens of kilowatts down to only a few watts. At multihundred watt unit size, the FPSE can be directly integrated with the General Purpose Heat Source (GPHS) via radiative coupling; the resulting dynamic isotope power system has a size and weight that compares favorably with the advanced modular (Mod) RTG, but requires less than a third the amount of isotope fuel. Thus the FPSE extends the high efficiency advantage of dynamic systems into a power range never previously considered competitive for DIPS. This results in lower fuel cost and reduced radiological hazard per delivered electrical watt.

Small Stirling dynamic isotope power system for multihundred-watt robotic missions

NASA Technical Reports Server (NTRS)

Bents, David J.

1991-01-01

Free piston Stirling Engine (FPSE) and linear alternator (LA) technology is combined with radioisotope heat sources to produce a compact dynamic isotope power system (DIPS) suitable for multihundred watt space application which appears competitive with advanced radioisotope thermoelectric generators (RTGs). The small Stirling DIPS is scalable to multihundred watt power levels or lower. The FPSE/LA is a high efficiency convertor in sizes ranging from tens of kilowatts down to only a few watts. At multihundred watt unit size, the FPSE can be directly integrated with the General Purpose Heat Source (GPHS) via radiative coupling; the resulting dynamic isotope power system has a size and weight that compares favorably with the advanced modular (Mod) RTG, but requires less than a third the amount of isotope fuel. Thus the FPSE extends the high efficiency advantage of dynamic systems into a power range never previously considered competitive for DIPS. This results in lower fuel cost and reduced radiological hazard per delivered electrical watt.

Multi-Isotopic evidence from West Eifel Xenoliths

NASA Astrophysics Data System (ADS)

Thiemens, M. M.; Sprung, P.

2015-12-01

Mantle Xenoliths from the West Eifel intraplate volcanic field of Germany provide insights into the nature and evolution of the regional continental lithospheric mantle. Previous isotope studies have suggested a primary Paleoproterozoic depletion age, a second partial melting event in the early Cambrian, and a Variscan metasomatic overprint. Textural and Sr-Nd isotopic observations further suggest two episodes of melt infiltration of early Cretaceous and Quaternary age. We have investigated anhydrous, vein-free lherzolites from this region, focusing on the Dreiser Weiher and Meerfelder Maar localities. Hand separated spinel, olivine, ortho- and clinopryoxene, along with host and bulk rocks were dissolved and purified for Rb-Sr, Sm-Nd, and Lu-Hf analysis on the Cologne/Bonn Neptune MC-ICP-MS. We find an unexpected discontinuity between mineral separates and whole rocks. While the latter have significantly more radiogenic ɛNd and ɛHf, mineral separates imply close-to chondritic compositions. Our Lu-Hf data imply resetting of the Lu-Hf systematic after 200 Ma. Given the vein-free nature of the lherzolites, this appears to date to the second youngest metasomatic episode. We suggest that markedly radiogenic Nd and Hf were introduced during the Quarternary metasomatic episode and most likely reside on grain boundaries.

Constraints on the origin of Os-isotope disequilibrium in included and interstitial sulfides in mantle peridotites: Implications for the interpretation of Os-isotope signatures in MORB and Abyssal Peridotites

NASA Astrophysics Data System (ADS)

Lassiter, J. C.

2016-12-01

The use of isotope variations in basalts to probe the composition and evolution of the mantle is predicated on the assumption of local (i.e., grain-scale) isotopic equilibrium during mantle melting (Hofmann & Hart, 1978). However, several studies report Os-isotope disequilibrium in distinct populations of sulfides in some peridotites. In principle, grain-scale isotopic heterogeneity could reflect variable radiogenic ingrowth in ancient sulfides with variable Re/Os, or partial re-equilibration of low-Re/Os sulfides with high-Re/Os silicate phases along grain boundaries during mantle melting (e.g., Alard et al., 2005). Both cases require that sulfides fail to maintain isotopic equilibrium with neighboring phases over geologically long ( Ga) time scales. The preservation of Os-isotope disequilibrium in peridotites has been ascribed to the armoring effect of low-[Os] silicates, which limit diffusive exchange between isolated Os-rich phases. This raises the prospect that peridotite-derived melts may not inherit the Os-isotope composition of their source. The timescale required for diffusive equilibration between separate sulfide grains or between Os-rich sulfides and Os-poor silicates is a function of average sulfide size and spacing, Os diffusivity in armoring silicate minerals, and Os partitioning between silicate and sulfide phases. For typical sulfide abundances and sizes in mantle peridotites, neighboring sulfides are expected to re-equilibrate in less than a few 10s of m.y. at adiabatic mantle temperatures, even for very high (>106) sulfide/silicate KD values. Maintenance of disequilibrium requires very large sulfides (>100 um) separated by several mm and diffusion rates (D < 10-20 m2/s) slower than for most other elements in olivine. Equilibration timescales between sulfides and surrounding silicates are similar, so that large-scale isotopic disequilibrium between sulfides and silicates is also unlikely within the convecting mantle. Instead, observed grain

Isotopic Discrimination During Leaf Litter Decomposition

NASA Astrophysics Data System (ADS)

Ngao, J.; Rubino, M.

2006-12-01

implement an advanced laser spectrometry technology to measure the isotopic composition in respired CO2. The laser spectrometer will be used to investigate the isotopic discrimination during soil respiration, in laboratory and field studies.

Advancing the Theory of Nuclear Reactions with Rare Isotopes. From the Laboratory to the Cosmos

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nunes, Filomena

2015-06-01

The mission of the Topical Collaboration on the Theory of Reactions for Unstable iSotopes (TORUS) was to develop new methods to advance nuclear reaction theory for unstable isotopes—particularly the (d,p) reaction in which a deuteron, composed of a proton and a neutron, transfers its neutron to an unstable nucleus. After benchmarking the state-of-the-art theories, the TORUS collaboration found that there were no exact methods to study (d,p) reactions involving heavy targets; the difficulty arising from the long-range nature of the well known, yet subtle, Coulomb force. To overcome this challenge, the TORUS collaboration developed a new theory where the complexitymore » of treating the long-range Coulomb interaction is shifted to the calculation of so-called form-factors. An efficient implementation for the computation of these form factors was a major achievement of the TORUS collaboration. All the new machinery developed are essential ingredients to analyse (d,p) reactions involving heavy nuclei relevant for astrophysics, energy production, and stockpile stewardship.« less

The oxygen isotope composition of Almahata Sitta

NASA Astrophysics Data System (ADS)

Rumble, Douglas; Zolensky, Michael E.; Friedrich, Jon M.; Jenniskens, Peter; Shaddad, Muawia H.

2010-10-01

Eleven fragments of the meteorite Almahata Sitta (AHS) have been analyzed for oxygen isotopes. The fragments were separately collected as individual stones from the meteorite's linear strewn field in the Nubian Desert. Each of the fragments represents a sample of a different and distinct portion of asteroid 2008 TC3. Ten of the fragments span the same range of values of δ18O, δ17O, and Δ17O, and follow the same trend along the carbonaceous chondrite anhydrous minerals (CCAM) line as monomict and polymict members of the ureilite family of meteorites. The oxygen isotope composition of fragment #25 is consistent with its resemblance petrographically to an H5 ordinary chondrite. Our results demonstrate that a single small asteroidal parent body, asteroid 2008 TC3, only 4 m in length, encompassed the entire range of variation in oxygen isotope compositions measured for monomict and polymict ureilites.

Application of stable isotope ratio analysis for biodegradation monitoring in groundwater

USGS Publications Warehouse

Hatzinger, Paul B.; Böhlke, John Karl; Sturchio, Neil C.

2013-01-01

Stable isotope ratio analysis is increasingly being applied as a tool to detect, understand, and quantify biodegradation of organic and inorganic contaminants in groundwater. An important feature of this approach is that it allows degradative losses of contaminants to be distinguished from those caused by non-destructive processes such as dilution, dispersion, and sorption. Recent advances in analytical techniques, and new approaches for interpreting stable isotope data, have expanded the utility of this method while also exposing complications and ambiguities that must be considered in data interpretations. Isotopic analyses of multiple elements in a compound, and multiple compounds in the environment, are being used to distinguish biodegradative pathways by their characteristic isotope effects. Numerical models of contaminant transport, degradation pathways, and isotopic composition are improving quantitative estimates of in situ contaminant degradation rates under realistic environmental conditions.

Design of an EBIS charge breeder system for rare-isotope beams

NASA Astrophysics Data System (ADS)

Park, Young-Ho; Son, Hyock-Jun; Kim, Jongwon

2016-09-01

Rare-isotope beams will be produced by using the isotope separation on-line (ISOL) system at the Rare Isotope Science Project (RISP). A proton cyclotron is the driver accelerator for ISOL targets, and uranium carbide (UCx) will be a major target material. An isotope beam of interest extracted from the target will be ionized and selected by using a mass separator. The beam emittance will then be reduced by using a radio-frequency quadrupole (RFQ) cooler before the beam is injected into the electron-beam ion-source (EBIS) charge breeder (CB). The maximum electron beam current of the EBIS is 3 A from a cathode made of IrCe in an applied magnetic field of 0.2 T. The size of the electron beam is compressed by magnetic fields of up to 6 T caused in the charge-breeding region by a superconducting solenoid. The design of EBIS-CB was performed by using mechanics as well as beam optics. A test stand for the electron gun and its collector, which can take an electron-beam power of 20 kW, are under construction. The gun assembly was first tested by using a high-voltage pulse so as to measure its perveance. The design of the EBIS, along with its test stand, is described.

Laser ablation inductively coupled plasma mass spectrometry for direct isotope ratio measurements on solid samples

NASA Astrophysics Data System (ADS)

Pickhardt, Carola; Dietze, Hans-Joachim; Becker, J. Sabine

2005-04-01

Isotope ratio measurements have been increasingly used in quite different application fields, e.g., for the investigation of isotope variation in nature, in geoscience (geochemistry and geochronology), in cosmochemistry and planetary science, in environmental science, e.g., in environmental monitoring, or by the application of the isotope dilution technique for quantification purposes using stable or radioactive high-enriched isotope tracers. Due to its high sensitivity, laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) is today a challenging mass spectrometric technique for the direct determination of precise and accurate isotope ratios in solid samples. In comparison to laser ablation quadrupole ICP-MS (LA-ICP-QMS), laser ablation coupled to a double-focusing sector field ICP-MS (LA-ICP-SFMS) with single ion detection offers a significant improvement of sensitivity at low mass resolution, whereby isotope ratios can be measured with a precision to 0.1% relative standard deviation (R.S.D.). In LA-ICP-SFMS, many disturbing isobaric interferences of analyte and molecular ions can be separated at the required mass resolution (e.g., 40Ar16O+ and 56Fe+ for iron isotope ratio measurements). The precision on isotope ratio measurements was improved by one order of magnitude via the simultaneous detection of mass-separated ion currents of isotopes using multiple ion collectors in LA-ICP-MS (LA-MC-ICP-MS). The paper discusses the state of the art, the challenges and limits in isotope ratio measurements by LA-ICP-MS using different instrumentations at the trace and ultratrace level in different fields of application as in environmental and biological research, geochemistry and geochronology with respect to their precision and accuracy.

The Radio Frequency Fragment Separator for Rare Isotope Beams at the NSCL

NASA Astrophysics Data System (ADS)

Stoker, Joshua; Andreev, Vladimir; Bazin, Daniel; Becerril, Ana; Doleans, Marc; Gorelov, Dimitry; Glennon, Patrick; Grimm, Terry; Lawton, Don; Mantica, Paul; Marti, Felix; Ottarson, Jack; Schatz, Hendrik; Vincent, John; Wagner, Jim; Wu, Xiaoyu; Zeller, Al

2006-10-01

Secondary beams at the National Superconducting Cyclotron Laboratory (NSCL) are separated through a combined application of magnetic rigidity and energy loss filtering. Design and construction of a Radio Frequency Fragment Separator (RFFS) for further beam purification is underway. The RFFS will apply a time-varying electromagnetic field to induce transverse beam separation. This method relies on velocity differences of the beam species to selectivey apply separation to unwanted fragments. The technical design of the RFFS and the expected purification of exotic beams are shown in detail[1]. [1] Gorelev, D. et al., ``RF Kicker System for Secondary Beams at the NSCL'' Proc of Part Accel Conf 2005, Knoxville, TN

Paleoproxies: Heavy Stable Isotope Perspectives

NASA Astrophysics Data System (ADS)

Nagler, T. F.; Hippler, D.; Siebert, C.; Kramers, J. D.

2002-12-01

Recent advances in isotope ratio mass spectrometry, namely multiple collector ICP-MS and refined TIMS techniques, will significantly enhance the ability to measure heavy stable isotope fractionation, which will lead to the development of a wide array of process-identifying (bio)-geochemical tools. Thus far research in this area is not easily assessable to scientists outside the isotope field. This is due to the fact that analyzing heavy stable isotopes does not provide routine numbers which are per se true (the preciser the truer) but is still a highly experimental field. On the other hand resolving earth science problems requires specialists familiar with the environment being studied. So what is in there for paleoceanographers? In a first order approach, relating isotope variations to physical processes is straightforward. A prominent example are oxygen isotope variations with temperature. The total geological signal is of course far more complicated. At low temperatures, heavy stable isotopes variations have been reported for e.g. Ca, Cr, Fe, Cu, Zn, Mo and Tl. Fractionation mechanisms and physical parameters responsible for the observed variations are not yet resolved for most elements. Significant equilibrium isotope fractionation is expected from redox reactions of transition metals. However a difference in coordination number between two coexisting speciations of an element in the same oxidation state can also cause fractionation. Protonation of dissolved Mo is one case currently discussed. For paleoceanography studies, a principal distinction between transition metals essential for life (V to Zn plus Mo) or not will be helpful. In case of the former group, distinction between biogenic and abiogenic isotope fractionation will remain an important issue. For example, abiotic Fe redox reactions result in isotope fractionations indistinguishable in direction and magnitude from microbial effects. Only a combination of different stable isotope systems bears the

Advances in high frequency ultrasound separation of particulates from biomass.

PubMed

Juliano, Pablo; Augustin, Mary Ann; Xu, Xin-Qing; Mawson, Raymond; Knoerzer, Kai

2017-03-01

In recent years the use of high frequency ultrasound standing waves (megasonics) for droplet or cell separation from biomass has emerged beyond the microfluidics scale into the litre to industrial scale applications. The principle for this separation technology relies on the differential positioning of individual droplets or particles across an ultrasonic standing wave field within the reactor and subsequent biomass material predisposition for separation via rapid droplet agglomeration or coalescence into larger entities. Large scale transducers have been characterised with sonochemiluminescence and hydrophones to enable better reactor designs. High frequency enhanced separation technology has been demonstrated at industrial scale for oil recovery in the palm oil industry and at litre scale to assist olive oil, coconut oil and milk fat separation. Other applications include algal cell dewatering and milk fat globule fractionation. Frequency selection depends on the material properties and structure in the biomass mixture. Higher frequencies (1 and 2MHz) have proven preferable for better separation of materials with smaller sized droplets such as milk fat globules. For palm oil and olive oil, separation has been demonstrated within the 400-600kHz region, which has high radical production, without detectable impact on product quality. Crown Copyright © 2016. Published by Elsevier B.V. All rights reserved.

Integrated Stable Isotope - Reactive Transport Model Approach for Assessment of Chlorinated Solvent Degradation

DTIC Science & Technology

2016-05-01

Certification Program ETH Ethene GC Gas Chromatography GC-IRMS Gas Chromatography Isotope Ratio Mass Spectroscopy H Hydrogen IRMS Isotope...tool for attenuation of chlorinated solvents. The Demonstration Site was Operable Unit 10 at Hill AFB, Utah , a site where groundwater is impacted...techniques. The method involves extraction of the target compounds from environmental sample matrix, followed by separation of the compounds using gas

Enzymatic Kinetic Isotope Effects from Path-Integral Free Energy Perturbation Theory.

PubMed

Gao, J

2016-01-01

Path-integral free energy perturbation (PI-FEP) theory is presented to directly determine the ratio of quantum mechanical partition functions of different isotopologs in a single simulation. Furthermore, a double averaging strategy is used to carry out the practical simulation, separating the quantum mechanical path integral exactly into two separate calculations, one corresponding to a classical molecular dynamics simulation of the centroid coordinates, and another involving free-particle path-integral sampling over the classical, centroid positions. An integrated centroid path-integral free energy perturbation and umbrella sampling (PI-FEP/UM, or simply, PI-FEP) method along with bisection sampling was summarized, which provides an accurate and fast convergent method for computing kinetic isotope effects for chemical reactions in solution and in enzymes. The PI-FEP method is illustrated by a number of applications, to highlight the computational precision and accuracy, the rule of geometrical mean in kinetic isotope effects, enhanced nuclear quantum effects in enzyme catalysis, and protein dynamics on temperature dependence of kinetic isotope effects. © 2016 Elsevier Inc. All rights reserved.

Advances in the Metrology of Absolute Value Assignments to Isotopic Reference Materials: Consequences from the Avogadro Project

NASA Astrophysics Data System (ADS)

Vocke, Robert; Rabb, Savelas

2015-04-01

All isotope amount ratios (hereafter referred to as isotope ratios) produced and measured on any mass spectrometer are biased. This unfortunate situation results mainly from the physical processes in the source area where ions are produced. Because the ionized atoms in poly-isotopic elements have different masses, such processes are typically mass dependent and lead to what is commonly referred to as mass fractionation (for thermal ionization and electron impact sources) and mass bias (for inductively coupled plasma sources.) This biasing process produces a measured isotope ratio that is either larger or smaller than the "true" ratio in the sample. This has led to the development of numerous fractionation "laws" that seek to correct for these effects, many of which are not based on the physical processes giving rise to the biases. The search for tighter and reproducible precisions has led to two isotope ratio measurement systems that exist side-by-side. One still seeks to measure "absolute" isotope ratios while the other utilizes an artifact based measurement system called a delta-scale. The common element between these two measurement systems is the utilization of isotope reference materials (iRMs). These iRMs are used to validate a fractionation "law" in the former case and function as a scale anchor in the latter. Many value assignments of iRMs are based on "best measurements" by the original groups producing the reference material, a not entirely satisfactory approach. Other iRMs, with absolute isotope ratio values, have been produced by calibrated measurements following the Atomic Weight approach (AW) pioneered by NBS nearly 50 years ago. Unfortunately, the AW is not capable of calibrating the new generation of iRMs to sufficient precision. So how do we get iRMs with isotope ratios of sufficient precision and without bias? Such a focus is not to denigrate the extremely precise delta-scale measurements presently being made on non-traditional and tradition

Long-term fertilization alters chemically-separated soil organic carbon pools: Based on stable C isotope analyses

PubMed Central

Dou, Xiaolin; He, Ping; Cheng, Xiaoli; Zhou, Wei

2016-01-01

Quantification of dynamics of soil organic carbon (SOC) pools under the influence of long-term fertilization is essential for predicting carbon (C) sequestration. We combined soil chemical fractionation with stable C isotope analyses to investigate the C dynamics of the various SOC pools after 25 years of fertilization. Five types of soil samples (0–20, 20–40 cm) including the initial level (CK) and four fertilization treatments (inorganic nitrogen fertilizer, IN; balanced inorganic fertilizer, NPK; inorganic fertilizer plus farmyard manure, MNPK; inorganic fertilizer plus corn straw residue, SNPK) were separated into recalcitrant and labile fractions, and the fractions were analysed for C content, C:N ratios, δ13C values, soil C and N recalcitrance indexes (RIC and RIN). Chemical fractionation showed long-term MNPK fertilization strongly increased the SOC storage in both soil layers (0–20 cm = 1492.4 gC m2 and 20–40 cm = 1770.6 gC m2) because of enhanced recalcitrant C (RC) and labile C (LC). The 25 years of inorganic fertilizer treatment did not increase the SOC storage mainly because of the offsetting effects of enhanced RC and decreased LC, whereas no clear SOC increases under the SNPK fertilization resulted from the fast decay rates of soil C. PMID:26750143

Hydrogen isotope exchange in a metal hydride tube

DOE Office of Scientific and Technical Information (OSTI.GOV)

Robinson, David B.

2014-09-01

This report describes a model of the displacement of one hydrogen isotope within a metal hydride tube by a different isotope in the gas phase that is blown through the tube. The model incorporates only the most basic parameters to make a clear connection to the theory of open-tube gas chromatography, and to provide a simple description of how the behavior of the system scales with controllable parameters such as gas velocity and tube radius. A single tube can be seen as a building block for more complex architectures that provide higher molar flow rates or other advanced design goals.

Precision mass measurements of neutron-rich Co isotopes beyond N =40

NASA Astrophysics Data System (ADS)

Izzo, C.; Bollen, G.; Brodeur, M.; Eibach, M.; Gulyuz, K.; Holt, J. D.; Kelly, J. M.; Redshaw, M.; Ringle, R.; Sandler, R.; Schwarz, S.; Stroberg, S. R.; Sumithrarachchi, C. S.; Valverde, A. A.; Villari, A. C. C.

2018-01-01

The region near Z =28 and N =40 is a subject of great interest for nuclear structure studies due to spectroscopic signatures in 68Ni suggesting a subshell closure at N =40 . Trends in nuclear masses and their derivatives provide a complementary approach to shell structure investigations via separation energies. Penning trap mass spectrometry has provided precise measurements for a number of nuclei in this region; however, a complete picture of the mass surfaces has so far been limited by the large uncertainty remaining for nuclei with N >40 along the iron (Z =26 ) and cobalt (Z =27 ) chains because these species are not available from traditional isotope separator online rare isotope facilities. The Low-Energy Beam and Ion Trap Facility at the National Superconducting Cyclotron Laboratory is the first and only Penning trap mass spectrometer coupled to a fragmentation facility and therefore presents the unique opportunity to perform precise mass measurements of these elusive isotopes. Here we present the first Penning trap measurements of Co,6968, carried out at this facility. Some ambiguity remains as to whether the measured values are ground-state or isomeric-state masses. A detailed discussion is presented to evaluate this question and to motivate future work. In addition, we perform ab initio calculations of ground-state and two-neutron separation energies of cobalt isotopes with the valence-space in-medium similarity renormalization group approach based on a particular set of two- and three-nucleon forces that predict saturation in infinite matter. We discuss the importance of these measurements and calculations for understanding the evolution of nuclear structure near 68Ni.

Integrated carbon and chlorine isotope modeling: applications to chlorinated aliphatic hydrocarbons dechlorination.

PubMed

Jin, Biao; Haderlein, Stefan B; Rolle, Massimo

2013-02-05

We propose a self-consistent method to predict the evolution of carbon and chlorine isotope ratios during degradation of chlorinated hydrocarbons. The method treats explicitly the cleavage of isotopically different C-Cl bonds and thus considers, simultaneously, combined carbon-chlorine isotopologues. To illustrate the proposed modeling approach we focus on the reductive dehalogenation of chlorinated ethenes. We compare our method with the currently available approach, in which carbon and chlorine isotopologues are treated separately. The new approach provides an accurate description of dual-isotope effects regardless of the extent of the isotope fractionation and physical characteristics of the experimental system. We successfully applied the new approach to published experimental results on dehalogenation of chlorinated ethenes both in well-mixed systems and in situations where mass-transfer limitations control the overall rate of biodegradation. The advantages of our self-consistent dual isotope modeling approach proved to be most evident when isotope fractionation factors of carbon and chlorine differed significantly and for systems with mass-transfer limitations, where both physical and (bio)chemical transformation processes affect the observed isotopic values.

Core formation conditons in planetesimals: constraints from isotope fractionation experiments.

NASA Astrophysics Data System (ADS)

Guignard, J.; Quitté, G.; Toplis, M. J.; Poitrasson, F.

2016-12-01

Planetesimals are small objects (10 to 1000 km) early accreted in the history of the solar system which show a wide variety of thermal history due to the initial amount of radiogenic elements [1] (26Al and 60Fe), from a simple metamorphism to a complete metal-silicate differentiation. Moreover, isotope compositions of siderophile element, e.g. Fe, Ni, and W in meteorites spread on a range that can be attributed to the process of core-mantle segregation. We therefore performed isotope fractionation experiments of nickel and tungsten between metal and silicate in a gas-mixing (CO-CO2) vertical furnace, at different temperatures (from 1270°C to 1600°C), oxygen fugacity (from IW+2 to IW-6) and annealing times (from 20 minutes to 48 hours). The starting silicate is an anorthite-diopside eutectic composition glass, synthesize from the respective oxides. The starting metal is either a nickel or tungsten wire according to the element to study. After each experiment, metal and silicate are mechanically separated and digested in acids. Nickel and Tungsten separation have been made according to the methods developed by [2] and [3] and isotopes measurements have been made using a high resolution MC-ICP-MS (Neptune; Thermofisher©). Results show evidence for a strong kinetic isotope fractionation during the first annealing times with a faster diffusion of lightest isotopes than heaviest. Similar mechanism has been already highlighted for iron isotope fractionation between silicate and metal [4]. Chemical and isotopic equilibrium is also reached in our experiments but the time required dependent on the conditions of temperature and oxygen fugacity. Therefore, at equilibrium, metal-silicate isotope fractionation has also been quantified as well its temperature dependence. These experimental data can be used in order to bring new constraints on the metal silicate segregation in the planetesimals early accreted. [1] Lee T., et al., GRL, 3, 41-44 (1976) [2] Quitté G., and Oberli

An isotope hydrology study of the Kilauea volcano area, Hawaii

USGS Publications Warehouse

Scholl, M.A.; Ingebritsen, S.E.; Janik, C.J.; Kauahikaua, J.P.

1995-01-01

Isotope tracer methods were used to determine flow paths, recharge areas, and relative age for ground water in the Kilauea volcano area on the Island of Hawaii. Stable isotopes in rainfall show three distinct isotopic gradients with elevation, which are correlated with trade-wind, rain shadow, and high-elevation climatological patterns. Temporal variations in isotopic composition of precipitation are controlled more by the frequency of large storms than b.y seasonal temperature fluctuations. Consistency in results between two separate areas with rainfall caused by tradewinds and thermally-driven upslope airflow suggests that isotopic gradients with elevation may be similar on other islands in the tradewind belt, especially the other Hawaiian Islands, which have similar climatology and temperature lapse rates. Areal contrasts in ground-water stable isotopes and tritium indicate that the volcanic ri~ zones compartmentalize the regional ground-water system. Tritium levels in ground water within and downgradient of Kilauea's ri~ zones indicate relatively long residence times. Part of Kilauea's Southwest Ri~ Zone appears to act as a conduit for water from higher elevation, but there is no evidence for extensive down-ri~ flow in the lower East Ri~ Zone.

Precise and accurate isotope ratio measurements by ICP-MS.

PubMed

Becker, J S; Dietze, H J

2000-09-01

The precise and accurate determination of isotope ratios by inductively coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS (LA-ICP-MS) is important for quite different application fields (e.g. for isotope ratio measurements of stable isotopes in nature, especially for the investigation of isotope variation in nature or age dating, for determining isotope ratios of radiogenic elements in the nuclear industry, quality assurance of fuel material, for reprocessing plants, nuclear material accounting and radioactive waste control, for tracer experiments using stable isotopes or long-lived radionuclides in biological or medical studies). Thermal ionization mass spectrometry (TIMS), which used to be the dominant analytical technique for precise isotope ratio measurements, is being increasingly replaced for isotope ratio measurements by ICP-MS due to its excellent sensitivity, precision and good accuracy. Instrumental progress in ICP-MS was achieved by the introduction of the collision cell interface in order to dissociate many disturbing argon-based molecular ions, thermalize the ions and neutralize the disturbing argon ions of plasma gas (Ar+). The application of the collision cell in ICP-QMS results in a higher ion transmission, improved sensitivity and better precision of isotope ratio measurements compared to quadrupole ICP-MS without the collision cell [e.g., for 235U/238U approximately 1 (10 microg x L(-1) uranium) 0.07% relative standard deviation (RSD) vs. 0.2% RSD in short-term measurements (n = 5)]. A significant instrumental improvement for ICP-MS is the multicollector device (MC-ICP-MS) in order to obtain a better precision of isotope ratio measurements (with a precision of up to 0.002%, RSD). CE- and HPLC-ICP-MS are used for the separation of isobaric interferences of long-lived radionuclides and stable isotopes by determination of spallation nuclide abundances in an irradiated tantalum target.

METHOD FOR PRODUCING ISOTOPIC METHANES FROM LITHIUM CARBONATE AND LITHIUM HYDRIDE

DOEpatents

Frazer, J.W.

1959-10-27

A process is descrlbed for the production of methane and for the production of methane containing isotopes of hydrogen and/or carbon. Finely divided lithium hydrlde and litldum carbonate reactants are mixed in intimate contact and subsequently compacted under pressures of from 5000 to 60,000 psl. The compacted lithium hydride and lithium carbenate reactunts are dispised in a gas collecting apparatus. Subsequently, the compact is heated to a temperature in the range 350 to 400 deg C whereupon a solid-solid reaction takes place and gaseous methane is evolved. The evolved methane is contaminated with gaseous hydrogen and a very small amount of CO/sub 2/; however, the desired methane product is separated from sald impurities by well known chemical processes, e.g., condensation in a cold trap. The product methane contalns isotopes of carbon and hydrogen, the Isotopic composition being determined by the carbon isotopes originally present In the lithium carbonate and the hydrogen isotopes originally present in the lithium hydride.

Quantifying dispersal rates and distances in North American martens: a test of enriched isotope labeling

Treesearch

Jonathan N. Pauli; Winston P. Smith; Merav Ben-David

2012-01-01

Advances in the application of stable isotopes have allowed the quantitative evaluation of previously cryptic ecological processes. In particular, researchers have utilized the predictable spatial patterning in natural abundance of isotopes to better understand animal dispersal and migration. However, quantifying dispersal via natural abundance alone has proven to be...

Process for recovering evolved hydrogen enriched with at least one heavy hydrogen isotope

DOEpatents

Tanaka, John; Reilly, Jr., James J.

1978-01-01

This invention relates to a separation means and method for enriching a hydrogen atmosphere with at least one heavy hydrogen isotope by using a solid titaniun alloy hydride. To this end, the titanium alloy hydride containing at least one metal selected from the group consisting of vanadium, chromium, manganese, molybdenum, iron, cobalt and nickel is contacted with a circulating gaseous flow of hydrogen containing at least one heavy hydrogen isotope at a temperature in the range of -20.degree. to +40.degree. C and at a pressure above the dissociation pressure of the hydrided alloy selectively to concentrate at least one of the isotopes of hydrogen in the hydrided metal alloy. The contacting is continued until equilibrium is reached, and then the gaseous flow is isolated while the temperature and pressure of the enriched hydride remain undisturbed selectively to isolate the hydride. Thereafter, the enriched hydrogen is selectively recovered in accordance with the separation factor (S.F.) of the alloy hydride employed.

13C metabolic flux analysis: optimal design of isotopic labeling experiments.

PubMed

Antoniewicz, Maciek R

2013-12-01

Measuring fluxes by 13C metabolic flux analysis (13C-MFA) has become a key activity in chemical and pharmaceutical biotechnology. Optimal design of isotopic labeling experiments is of central importance to 13C-MFA as it determines the precision with which fluxes can be estimated. Traditional methods for selecting isotopic tracers and labeling measurements did not fully utilize the power of 13C-MFA. Recently, new approaches were developed for optimal design of isotopic labeling experiments based on parallel labeling experiments and algorithms for rational selection of tracers. In addition, advanced isotopic labeling measurements were developed based on tandem mass spectrometry. Combined, these approaches can dramatically improve the quality of 13C-MFA results with important applications in metabolic engineering and biotechnology. Copyright © 2013 Elsevier Ltd. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hitchcock, D.; Colon-Mercado, H.; Krentz, T.

Hydrogen isotope separation is critical to the DOE’s mission in environmental remediation and nuclear nonproliferation. Isotope separation is also a critical technology for the NNSA, and the ability to perform the separations at room temperature with a relatively small amount of power and space would be a major advancement for their respective missions. Recent work has shown that 2-D materials such as graphene and hexagonal boron nitride can act as an isotopic sieve at room temperature; efficiently separating hydrogen isotopes in water with reported separation ratios of 10:1 for hydrogen: deuterium separation for a single pass. The work performed heremore » suggests that this technique has merit, and furthermore, we are investigating optimization and scale up of the required 2-D material based membranes.« less

The chemical and isotopic differentiation of an epizonal magma body: Organ Needle pluton, New Mexico

USGS Publications Warehouse

Verplanck, P.L.; Farmer, G.L.; McCurry, M.; Mertzman, S.A.

1999-01-01

Major and trace element, and Nd and Sr isotopic compositions of whole rocks and mineral separates from the Oligocene, alkaline Organ Needle pluton (ONP), southern New Mexico, constrain models for the differentiation of the magma body parental to this compositionally zoned and layered epizonal intrusive body. The data reveal that the pluton is rimmed by lower ??(Nd) (~-5) and higher 87Sr/86Sr (~0.7085) syenitic rocks than those in its interior (??(Nd) ~ 2, 87Sr/86Sr ~0.7060) and that the bulk compositions of the marginal rocks become more felsic with decreasing structural depth. At the deepest exposed levels of the pluton, the ??(Nd)~-5 lithology is a compositionally heterogeneous inequigranular syenite. Modal, compositional and isotopic data from separates of rare earth element (REE)-bearing major and accesory mineral phases (hornblende, titanite, apatite, zircon) demonstrate that this decoupling of trace and major elements in the inequigranular syenite results from accumulation of light REE (LREE)-bearing minerals that were evidently separated from silicic magmas as the latter rose along the sides of the magma chamber. Chemical and isotopic data for microgranular mafic enclaves, as well as for restite xenoliths of Precambrian granite wall rock, indicate that the isotopic distinction between the marginal and interior facies of the ONP probably reflects assimilation of the wall rock by ??(Nd) ~-2 mafic magmas near the base of the magma system. Fractional crystallization and crystal liquid separation of the crystally contaminated magma at the base and along the margins of the chamber generated the highly silicic magmas that ultimately pooled at the chamber top.

Development of fast-release solid catchers for rare isotopes

NASA Astrophysics Data System (ADS)

Nolen, Jerry; Greene, John; Elam, Jeffrey; Mane, Anil; Sampathkumaran, Uma; Winter, Raymond; Hess, David; Mushfiq, Mohammad; Stracener, Daniel; Wiendenhoever, Ingo

2015-04-01

Porous solid catchers of rare isotopes are being developed for use at high power heavy ion accelerator facilities such as RIKEN, FRIB, and RISP. Compact solid catchers are complementary to helium gas catchers for parasitic harvesting of rare isotopes in the in-flight separators. They are useful for short lived isotopes for basic nuclear physics research and longer-lived isotopes for off-line applications. Solid catchers can operate effectively with high intensity secondary beams, e.g. >> 1E10 atoms/s with release times as short as 10-100 milliseconds. A new method using a very sensitive and efficient RGA has been commissioned off-line at Argonne and is currently being shipped to Florida State University for in-beam measurements of the release curves using stable beams. The same porous solid catcher technology is also being evaluated for use in targets for the production of medical isotopes such as 211-At. Research supported by the U.S. DOE Office of Nuclear Physics under the SBIR Program and Contract # DE-AC02-06CH11357 and a University of Chicago Comprehensive Cancer Center/ANL Pilot Project.

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.

Advances in Methane Isotope Measurements via Direct Absorption Spectroscopy with Applications to Oil and Gas Source Characterization

NASA Astrophysics Data System (ADS)

Yacovitch, T. I.; Herndon, S. C.; Roscioli, J. R.; Petron, G.; Shorter, J. H.; Jervis, D.; McManus, J. B.; Nelson, D. D.; Zahniser, M. S.; Kolb, C. E., Jr.

2015-12-01

Instrumental developments in the measurement of multiple isotopes of methane (12CH4, 13CH4 and 12CH3D) are presented. A first generation 8-micron instrument quantifies 12CH4 and 13CH4 at a 1-second rate via tunable infrared direct absorption spectroscopy (TILDAS). A second generation instrument uses two 3-micron intraband cascade lasers in an Aerodyne dual laser chassis for simultaneous measurement of 12CH4, 13CH4 and 12CH3D. Sensitivity and noise performance improvements are examined. The isotopic signature of methane provides valuable information for emission source identification of this greenhouse gas. A first generation spectrometer has been deployed in the field on a mobile laboratory along with a sophisticated 4-tank calibration system. Calibrations are done on an agressive schedule, allowing for the correction of measured isotope ratios to an absolute isotope scale. Distinct isotopic signatures are found for a number of emission sources in the Denver-Julesburg Basin: oil and gas gathering stations, compressor stations and processing plants; a municipal landfill, and dairy/cattle operations. The isotopic signatures are compared with measured ethane/methane ratios. These direct absorption measurements have larger uncertainties than samples measured via gas chromatography-mass spectrometry, but have several advantages over canister sampling methods: individual sources of short duration are easier to isolate; calibrated isotope ratio results are available immediately; replicate measurements on a single source are easily performed; and the number of sources sampled is not limited by canister availability and processing time.

Water isotope systematics: Improving our palaeoclimate interpretations

USGS Publications Warehouse

Jones, M. D.; Dee, S.; Anderson, L.; Baker, A.; Bowen, G.; Noone, D.

2016-01-01

implications of advances in understanding in these areas for the interpretation of palaeo records and proxy data – climate model comparison.Here, we briefly review these areas of research, and discuss challenges for the water isotope community in improving our ability to partition climate vs. auxiliary signals in palaeoclimate data.

Identification of neutron deficient niobium, molybdenum and technetium isotopes

NASA Astrophysics Data System (ADS)

Gross, C. J.

We report on the in-beam identification of fourteen new isotopes in the A=80-90 region. Heavy-ion reactions with a recoil separator or charged particle and neutron detectors provided identification of γ-rays from these new niobium, molybdenum, and technetium isotopes. The procedures used are described and energy level systematics are discussed. The energy levels appear to be organized into rotational bands in nuclei with N≤44 while those with N ≥ 46 have more single-particle-like transitions. Lifetime measurements in 87Mo and 87Nb indicate that g {9}/{2} particle alignment strongly influences the collectivity of these nuclei.

Femtosecond Laser Ablation Multicollector ICPMS Analysis of Uranium Isotopes in NIST Glass

DOE Office of Scientific and Technical Information (OSTI.GOV)

Duffin, Andrew M.; Springer, Kellen WE; Ward, Jesse D.

We have utilized femtosecond laser ablation coupled to multi-collector inductively couple plasma mass spectrometry to measure the uranium isotopic content of NIST 61x (x=0,2,4,6) glasses. The uranium content of these glasses is a linear two-component mixing between isotopically natural uranium and the isotopically depleted spike used in preparing the glasses. Laser ablation results match extremely well, generally within a few ppm, with solution analysis following sample dissolution and chemical separation. In addition to isotopic data, sample utilization efficiency measurements indicate that over 1% of ablated uranium atoms reach a mass spectrometer detector, making this technique extremely efficient. Laser sampling alsomore » allows for spatial analysis and our data indicate that rare uranium concentration inhomogeneities exist in NIST 616 glass.« less

Isotope dilution inductively coupled plasma quadrupole mass spectrometry in connection with a chromatographic separation for ultra trace determinations of platinum group elements (Pt, Pd, Ru, Ir) in environmental samples.

PubMed

Müller, M; Heumann, K G

2000-09-01

An isotope dilution inductively coupled plasma quadrupole mass spectrometric (ID-ICP-QMS) method was developed for the simultaneous determination of the platinum group elements Pt, Pd, Ru, and Ir in environmental samples. Spike solutions, enriched with the isotopes 194Pt, 108Pd, 99Ru, and 191Ir, were used for the isotope dilution step. Interfering elements were eliminated by chromatographic separation using an anion-exchange resin. Samples were dissolved with aqua regia in a high pressure asher. Additional dissolution of possible silicate portions by hydrofluoric acid was usually not necessary. Detection limits of 0.15 ng x g(-1), 0.075 ng x g(-1), and 0.015 ng x g(-1) were achieved for Pt, Pd, Ru, and Ir, respectively, using sample weights of only 0.2 g. The reliability of the ID-ICP-QMS method was demonstrated by analyzing a Canadian geological reference material and by participating in an interlaboratory study for the determination of platinum and palladium in a homogenized road dust sample. Surface soil, sampled at different distances from a highway, showed concentrations in the range of 0.1-87 ng x g(-1). An exponential decrease of the platinum and palladium concentration with increasing distance and a small anthropogenic contribution to the natural background concentration of ruthenium and iridium was found in these samples.

Environmental Forensics: Using Compound-Specific Stable Carbon Isotope Analysis to Track Petroleum Contamination

NASA Astrophysics Data System (ADS)

Imfeld, A.; Ouellet, A.; Gelinas, Y.

2016-12-01

Crude oil and petroleum products are continually being introduced into the environment during transportation, production, consumption and storage. Source identification of these organic contaminants proves challenging due to a variety of factors; samples tend to be convoluted, compounds need to be separated from an unresolved complex mixtures of highly altered aliphatic and aromatic compounds, and chemical composition and biomarker distributions can be altered by weathering, aging, and degradation processes. The aim of our research is to optimize a molecular and isotopic (δ13C, δ2H) method to fingerprint and identify petroleum contaminants in soil and sediment matrices, and to trace the temporal and spatial extent of the contamination event. This method includes the extraction, separation and analysis of the petroleum derived hydrocarbons. Sample extraction and separation is achieved using sonication, column chromatography and urea adduction. Compound identification and molecular/isotopic fingerprinting is obtained by gas chromatography with flame ionization (GC-FID) and mass spectrometer (GC-MS) detection, as well as gas chromatography coupled to an isotope ratio mass spectrometer (GC-IRMS). This method will be used to assist the Centre d'Expertise en Analyse Environnementale du Québec to determine the nature, sources and timing of contamination events as well as for investigating the residual contamination involving petroleum products.

Isotope ratio mass spectrometry in nutrition research

DOE Office of Scientific and Technical Information (OSTI.GOV)

Luke, A.H.

Many of the biochemical pathways and processes that form the foundation of modern nutrition research was elucidated using stable isotopes as physiological tracers. Since the discovery of stable isotopes, improvements and innovations in mass spectrometry and chromatography have led to greatly expanded applications. This research project was designed to evaluate gas chromatography/combustion/isotope ratio mass spectrometry (GC/C/IRMS) as a tool for isotopic tracer studies and to delineate the operational parameters for the analysis of {sup 13}C-labeled cholesterol, leucine and {alpha}-ketoisocaproate. The same isotope ratio mass spectrometer was then used as the base instrument for the ratio mass spectrometer was then usedmore » as the base instrument for the development of two additional inlet systems: a continuous-flow inlet for the analyses of {sup 13}C and {sup 18}O as CO{sub 2} and a filament inlet for on-line combustion and isotopic analysis of non-volatile organic compounds. Each of these three inlets was evaluated and their utility in nutrition research illustrated. GC/C/IRMS was used to analyze cholesterol, leucine and {alpha}-ketoisocaproate with good accuracy, precision and little isotopic memory. For all three compounds the detection limits achieved well surpassed currently used technologies. For compounds that can be well separated by GC, GC/C/IRMS is a valuable analytical tool. The continuous-flow inlet provided good accuracy and precision for measurements of {sup 13}CO{sub 2} from breath tests and {sup 18}O as CO{sub 2} from total energy expenditure tests. Most importantly, the continuous-flow inlet increased sample throughput by at least a factor of three over conventional analytical techniques. The filament inlet provided accurate and precise {sup 13}C ratio measurements of both natural abundance and enriched standards of non-volatile organic compounds of physiological interest.« less

Sulfur and Hydrogen Isotope Anomalies in Organic Compounds from the Murchison Meteorite

NASA Technical Reports Server (NTRS)

Cooper, G. W.; Thiemens, M. H.; Jackson, T.; Chang, Sherwood

1996-01-01

Isotopic measurements have been made on organic sulfur and phosphorus compounds recently discovered in the Murchison meteorite. Carbon, hydrogen and sulfur measurements were performed on individual members of the organic sulfur compounds, alkyl sulfonates; and carbon and hydrogen measurements were made on bulk alkyl phosphonates. Cooper and Chang reported the first carbon isotopic measurements of Murchison organic sulfonates, providing insight into the potential synthetic mechanisms of these and, possibly, other organic species. Hydrogen isotopic measurements of the sulforiates now reveal deuterium excesses ranging from +660 to +2730 %. The deuterium enrichments indicate formation of the hydrocarbon portion of these compounds in a low temperature astrophysical environment consistent with that of dense molecular clouds. Measurements of the sulfur isotopes provide further constraints on the origin and mechanism of formation of these organic molecules. Recently, there has been growing documentation of sulfur isotopic anomalies in meteoritic material. Thiemens and Jackson have shown that some bulk ureilites possess excess S-33 and Thiemens et al. have reported excess S-33 in an oldhamite separate from the Norton County meteorite. Rees and Thode reported a large S-33 excess in an Allende acid residue, however, attempts to verify this measurements have been unsuccessful, possibly due to the heterogeneous nature of the carrier phase. With the recognition that sulfur isotopes may reflect chemistry in the protosolar nebula or the precursor molecular cloud, identification of potential carriers is of considerable interest. In the present study, the stable isotopes of sulfur were measured in methane sulfonic acid extracted from the Murchison meteorite. The isotopic composition was found to be: (delta)S-33 = 2.48 %, (delta)S-34 = 2.49 % and (delta)S-36 = 6.76 %. Based upon analysis of more than 60 meteoritic and numerous terrestrial samples, the mass fractionation lines are

Investigation related to hydrogen isotopes separation by cryogenic distillation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bornea, A.; Zamfirache, M.; Stefanescu, I.

2008-07-15

Research conducted in the last fifty years has shown that one of the most efficient techniques of removing tritium from the heavy water used as moderator and coolant in CANDU reactors (as that operated at Cernavoda (Romania)) is hydrogen cryogenic distillation. Designing and implementing the concept of cryogenic distillation columns require experiments to be conducted as well as computer simulations. Particularly, computer simulations are of great importance when designing and evaluating the performances of a column or a series of columns. Experimental data collected from laboratory work will be used as input for computer simulations run at larger scale (formore » The Pilot Plant for Tritium and Deuterium Separation) in order to increase the confidence in the simulated results. Studies carried out were focused on the following: - Quantitative analyses of important parameters such as the number of theoretical plates, inlet area, reflux flow, flow-rates extraction, working pressure, etc. - Columns connected in series in such a way to fulfil the separation requirements. Experiments were carried out on a laboratory-scale installation to investigate the performance of contact elements with continuous packing. The packing was manufactured in our institute. (authors)« less

Development of high through-put Sr isotope analysis for monitoring reservoir integrity for CO{sub 2} storage.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wall, Andy; Jain, Jinesh; Stewart, Brian

2012-01-01

Recent innovations in multi-collector ICP-mass spectrometry (MC-ICP-MS) have allowed for rapid and precise measurements of isotope ratios in geological samples. Naturally occurring Sr isotopes has the potential for use in Monitoring, Verification, and Accounting (MVA) associated with geologic CO2 storage. Sr isotopes can be useful for: Sensitive tracking of brine migration; Determining seal rock leakage; Studying fluid/rock reactions. We have optimized separation chemistry procedures that will allow operators to prepare samples for Sr isotope analysis off site using rapid, low cost methods.

Stable isotope-resolved metabolomics and applications for drug development

PubMed Central

Fan, Teresa W-M.; Lorkiewicz, Pawel; Sellers, Katherine; Moseley, Hunter N.B.; Higashi, Richard M.; Lane, Andrew N.

2012-01-01

Advances in analytical methodologies, principally nuclear magnetic resonance spectroscopy (NMR) and mass spectrometry (MS), during the last decade have made large-scale analysis of the human metabolome a reality. This is leading to the reawakening of the importance of metabolism in human diseases, particularly cancer. The metabolome is the functional readout of the genome, functional genome, and proteome; it is also an integral partner in molecular regulations for homeostasis. The interrogation of the metabolome, or metabolomics, is now being applied to numerous diseases, largely by metabolite profiling for biomarker discovery, but also in pharmacology and therapeutics. Recent advances in stable isotope tracer-based metabolomic approaches enable unambiguous tracking of individual atoms through compartmentalized metabolic networks directly in human subjects, which promises to decipher the complexity of the human metabolome at an unprecedented pace. This knowledge will revolutionize our understanding of complex human diseases, clinical diagnostics, as well as individualized therapeutics and drug response. In this review, we focus on the use of stable isotope tracers with metabolomics technologies for understanding metabolic network dynamics in both model systems and in clinical applications. Atom-resolved isotope tracing via the two major analytical platforms, NMR and MS, has the power to determine novel metabolic reprogramming in diseases, discover new drug targets, and facilitates ADME studies. We also illustrate new metabolic tracer-based imaging technologies, which enable direct visualization of metabolic processes in vivo. We further outline current practices and future requirements for biochemoinformatics development, which is an integral part of translating stable isotope-resolved metabolomics into clinical reality. PMID:22212615

Production of platinum radioisotopes at Brookhaven Linac Isotope Producer (BLIP)

DOE PAGES

Smith, Suzanne V.; Mccutchan, Elizabeth; Gurdal, Gulhan; ...

2017-09-13

The accelerator production of platinum isotopes was investigated at the Brookhaven Linac Isotope Producer (BLIP). In this paper high purity natural platinum foils were irradiated at 53.2, 65.7, 105.2, 151.9, 162.9 and 173.3 MeV. The irradiated foils were digested in aqua regia and then converted to their hydrochloride salt with concentrated hydrochloric acid before analyzing by gamma spectrometry periodically for at least 10 days post end of bombardment. A wide range of platinum (Pt), gold (Au) and iridiu m (Ir) isotopes were identified. Effective cross sections at BLIP for Pt-188, Pt-189, Pt-191 and Pt-195m were compared to literature and theoreticalmore » cross sections determined using Empire-3.2. The majority of the effective cross sections (<70 MeV) confirm those reported in the literature. While the absolute values of the theoretical cross sections were up to a factor of 3 lower, Empire 3.2 modeled thresholds and maxima correlated well with experimental values. Preliminary evaluation into a rapid separation of Pt isotopes from high levels of Ir and Au isotopes proved to be a promising approach for large scale production. In conclusion, this study demonstrated that with the use of isotopically enriched target material accelerator production of selected platinum isotopes is feasible over a wide proton energy range.« less

Production of platinum radioisotopes at Brookhaven Linac Isotope Producer (BLIP)

NASA Astrophysics Data System (ADS)

Smith, Suzanne V.; McCutchan, Elizabeth; Gürdal, Gülhan; Lister, Christopher; Muench, Lisa; Nino, Michael; Sonzogni, Alexandro; Herman, Michal; Nobre, Gustavo; Cullen, Chris; Chillery, Thomas; Chowdury, Partha; Harding, Robert

2017-09-01

The accelerator production of platinum isotopes was investigated at the Brookhaven Linac Isotope Producer (BLIP). In this study high purity natural platinum foils were irradiated at 53.2, 65.7, 105.2, 151.9, 162.9 and 173.3.MeV. The irradiated foils were digested in aqua regia and then converted to their hydrochloride salt with concentrated hydrochloric acid before analyzing by gamma spectrometry periodically for at least 10 days post end of bombardment. A wide range of platinum (Pt), gold (Au) and iridium (Ir) isotopes were identified. Effective cross sections at BLIP for Pt-188, Pt-189, Pt-191 and Pt-195m were compared to literature and theoretical cross sections determined using Empire-3.2. The majority of the effective cross sections (<70 MeV) confirm those reported in the literature. While the absolute values of the theoretical cross sections were up to a factor of 3 lower, Empire 3.2 modeled thresholds and maxima correlated well with experimental values. Preliminary evaluation into a rapid separation of Pt isotopes from high levels of Ir and Au isotopes proved to be a promising approach for large scale production. In conclusion, this study demonstrated that with the use of isotopically enriched target material accelerator production of selected platinum isotopes is feasible over a wide proton energy range.

Re-Os isotopic systematics in chromitites from the Stillwater Complex, Montana, USA

NASA Astrophysics Data System (ADS)

Marcantonio, Franco; Zindler, Alan; Reisberg, Laurie; Mathez, E. A.

1993-08-01

New Re-Os isotopic data on chromitites of the Stillwater Complex demonstrate isotopic equilibrium between cumulate chromite and whole rock. Initial osmium isotopic ratios for the chromitites, chosen for their freshness, are consistent with derivation from a mantle-derived magma that suffered little or no interaction with the continental crust prior to crystallization. Molybdenite, separated from a sample of the G-chromitite, yields a Re-Os age of 2740 Ma, indistinguishable from the age of the intrusion. The presence of molybdenite documents rhenium, and probably osmium, mobilization by hydrothermal fluids that permeated the intrusion shortly after crystallization. Initial osmium isotopic variability observed in chromitites and other rocks from the Stillwater Complex could result from interaction with these fluids. In this context, there is no compelling reason to call on assimilation of crust by mantle-derived magma to explain the osmium or neodymium isotopic variability. Although osmium isotopic systematics have been affected by hydrothermal processes, Re-Os results demonstrate that more than 95 percent of the osmium, and by inference other PGEs in the Stillwater Complex, derive from the mantle.

Identifying the groundwater basin boundaries, using environmental isotopes: a case study

NASA Astrophysics Data System (ADS)

Demiroğlu, Muhterem

2017-06-01

Groundwater, which is renewable under current climatic conditions separately from other natural sources, in fact is a finite resource in terms of quality and fossil groundwater. Researchers have long emphasized the necessity of exploiting, operating, conserving and managing groundwater in an efficient and sustainable manner with an integrated water management approach. The management of groundwater needs reliable information about changes on groundwater quantity and quality. Environmental isotopes are the most important tools to provide this support. No matter which method we use to calculate the groundwater budget and flow equations, we need to determine boundary conditions or the physical boundaries of the domain. The Groundwater divide line or basin boundaries that separate the two adjacent basin recharge areas from each other must be drawn correctly to be successful in defining complex groundwater basin boundary conditions. Environmental isotope data, as well as other methods provide support for determining recharge areas of the aquifers, especially for karst aquifers, residence time and interconnections between aquifer systems. This study demonstrates the use of environmental isotope data to interpret and correct groundwater basin boundaries giving as an example the Yeniçıkrı basin within the main Sakarya basin.

Developing the Molybdenum Isotopic Proxy in Marine Barite

NASA Astrophysics Data System (ADS)

Erhardt, A. M.; Paytan, A.; Aggarwal, J.

2006-12-01

Molybdenum isotope ratios in seawater fluctuate in response to changing redox conditions and can provide clues into the degree of global ocean anoxia. The isotopic ratio of molybdenum has been shown to be sensitive to the relative proportion of oxic, suboxic, and euxinic environments. Deposition in oxic environments is isotopically light (~ -1.6‰ for δ^{97/95}Mo) relative to an average crustal source (0‰). Conversely, euxinic environments have been shown to be consistently heavier (~1.3‰) than the oxic sink through time, with suboxic sediments falling between these two signals. Shifts in the relative proportion of each sink, relative to a constant source, would alter the isotopic ratio of seawater over long time scales. Previously, this seawater value, and hence the degree of global anoxia, could only be inferred through mass balance calculations. We seek to quantify the isotopic signature of seawater though time using a phase that directly records this ratio. Marine barite precipitates inorganically in the water column directly from seawater, potentially providing a direct record of seawater characteristics. Molybdenum is a trace constituent of barite, with the molybdate ion substituting for sulfate at concentrations of about 1 ppm. To accurately determine the molybdenum isotopic ratio at these low concentrations (<15 ng per sample), modifications to existing measurement techniques are required. We will present the variations made to existing separation and mass-spectrometry techniques and the calibration of these new methods. The modifications were undertaken to reduce molybdenum blank to below 1 ng per analysis, to quantitatively remove interfering zirconium and to measure precise and reproducible isotope values. Preliminary data will be presented to illustrate potential applications for this new paleoredox proxy. This technique will allow for the measurement of molybdenum isotopic ratios at low concentrations, expanding the breath of compounds and

Application of Stable Isotope-Assisted Metabolomics for Cell Metabolism Studies

PubMed Central

You, Le; Zhang, Baichen; Tang, Yinjie J.

2014-01-01

The applications of stable isotopes in metabolomics have facilitated the study of cell metabolisms. Stable isotope-assisted metabolomics requires: (1) properly designed tracer experiments; (2) stringent sampling and quenching protocols to minimize isotopic alternations; (3) efficient metabolite separations; (4) high resolution mass spectrometry to resolve overlapping peaks and background noises; and (5) data analysis methods and databases to decipher isotopic clusters over a broad m/z range (mass-to-charge ratio). This paper overviews mass spectrometry based techniques for precise determination of metabolites and their isotopologues. It also discusses applications of isotopic approaches to track substrate utilization, identify unknown metabolites and their chemical formulas, measure metabolite concentrations, determine putative metabolic pathways, and investigate microbial community populations and their carbon assimilation patterns. In addition, 13C-metabolite fingerprinting and metabolic models can be integrated to quantify carbon fluxes (enzyme reaction rates). The fluxome, in combination with other “omics” analyses, may give systems-level insights into regulatory mechanisms underlying gene functions. More importantly, 13C-tracer experiments significantly improve the potential of low-resolution gas chromatography-mass spectrometry (GC-MS) for broad-scope metabolism studies. We foresee the isotope-assisted metabolomics to be an indispensable tool in industrial biotechnology, environmental microbiology, and medical research. PMID:24957020

In-Gel Stable-Isotope Labeling (ISIL): a strategy for mass spectrometry-based relative quantification.

PubMed

Asara, John M; Zhang, Xiang; Zheng, Bin; Christofk, Heather H; Wu, Ning; Cantley, Lewis C

2006-01-01

Most proteomics approaches for relative quantification of protein expression use a combination of stable-isotope labeling and mass spectrometry. Traditionally, researchers have used difference gel electrophoresis (DIGE) from stained 1D and 2D gels for relative quantification. While differences in protein staining intensity can often be visualized, abundant proteins can obscure less abundant proteins, and quantification of post-translational modifications is difficult. A method is presented for quantifying changes in the abundance of a specific protein or changes in specific modifications of a protein using In-gel Stable-Isotope Labeling (ISIL). Proteins extracted from any source (tissue, cell line, immunoprecipitate, etc.), treated under two experimental conditions, are resolved in separate lanes by gel electrophoresis. The regions of interest (visualized by staining) are reacted separately with light versus heavy isotope-labeled reagents, and the gel slices are then mixed and digested with proteases. The resulting peptides are then analyzed by LC-MS to determine relative abundance of light/heavy isotope pairs and analyzed by LC-MS/MS for identification of sequence and modifications. The strategy compares well with other relative quantification strategies, and in silico calculations reveal its effectiveness as a global relative quantification strategy. An advantage of ISIL is that visualization of gel differences can be used as a first quantification step followed by accurate and sensitive protein level stable-isotope labeling and mass spectrometry-based relative quantification.

Opinion: Why we need a centralized repository for isotopic data

USGS Publications Warehouse

Pauli, Jonathan N.; Newsome, Seth D.; Cook, Joseph A.; Harrod, Chris; Steffan, Shawn A.; Baker, Christopher J. O.; Ben-David, Merav; Bloom, David; Bowen, Gabriel J.; Cerling, Thure E.; Cicero, Carla; Cook, Craig; Dohm, Michelle; Dharampal, Prarthana S.; Graves, Gary; Gropp, Robert; Hobson, Keith A.; Jordan, Chris; MacFadden, Bruce; Pilaar Birch, Suzanne; Poelen, Jorrit; Ratnasingham, Sujeevan; Russell, Laura; Stricker, Craig A.; Uhen, Mark D.; Yarnes, Christopher T.; Hayden, Brian

2017-01-01

Stable isotopes encode and integrate the origin of matter; thus, their analysis offers tremendous potential to address questions across diverse scientific disciplines (1, 2). Indeed, the broad applicability of stable isotopes, coupled with advancements in high-throughput analysis, have created a scientific field that is growing exponentially, and generating data at a rate paralleling the explosive rise of DNA sequencing and genomics (3). Centralized data repositories, such as GenBank, have become increasingly important as a means for archiving information, and “Big Data” analytics of these resources are revolutionizing science and everyday life.

Isotopic Equilibrium in Mature Oceanic Lithosphere: Insights From Sm-Nd Isotopes on the Corsica (France) Ophiolites

NASA Astrophysics Data System (ADS)

Rampone, E.; Hofmann, A. W.; Raczek, I.; Romairone, A.

2003-12-01

In mature oceanic lithosphere, formed at mid-ocean ridges, residual mantle peridotites and associated magmatic crust are, in principle, linked by a cogenetic relationship, because the times of asthenospheric mantle melting and magmatic crust production are assumed to be roughly coheval. This implies that oceanic peridotites and associated magmatic rocks should have similar isotopic compositions. Few isotope studies have been devoted to test this assumption. At mid-ocean ridges, similar Nd isotopic compositions in basalts and abyssal peridotites have been found by Snow et al. (1994), thus indicating that oceanic peridotites are indeed residues of MORB melting. By contrast, Salters and Dick (2002) have documented Nd isotope differences between abyssal peridotites and associated basalts, with peridotites showing higher 143Nd/144Nd values, and they concluded that an enriched pyroxenitic source component is required to explain the low end of the 143Nd/144Nd variation of the basalts. Here we present Sm/Nd isotope data on ophiolitic mantle peridotites and intruded gabbroic rocks from Mt.Maggiore (Corsica, France), interpreted as lithosphere remnants of the Jurassic Ligurian Tethys ocean. The peridotites are residual after low-degree (<10%) fractional melting. In places, spinel peridotites grade to plagioclase-rich impregnated peridotites. Clinopyroxene separates from both spinel- and plagioclase- peridotites display high 147Sm/144Nd (0.49-0.59) and 143Nd/144Nd (0.513367-0.513551) ratios, consistent with their depleted signature. The associated gabbros have Nd isotopic compositions typical of MORB (143Nd/144Nd = 0.51312-0.51314). Sm/Nd data on plag, whole rock and cpx from an olivine gabbro define an internal isochron with an age of 162 +/- 10 Ma, and an initial epsilon Nd value (9.0) indicating a MORB-type source. In the Sm-Nd isochron diagram, the peridotite data also conform to the above linear array, their initial (160 Ma) epsilon Nd values varying in the range 7

Separation Potential for Multicomponent Mixtures: State-of-the Art of the Problem

NASA Astrophysics Data System (ADS)

Sulaberidze, G. A.; Borisevich, V. D.; Smirnov, A. Yu.

2017-03-01

Various approaches used in introducing a separation potential (value function) for multicomponent mixtures have been analyzed. It has been shown that all known potentials do not satisfy the Dirac-Peierls axioms for a binary mixture of uranium isotopes, which makes their practical application difficult. This is mainly due to the impossibility of constructing a "standard" cascade, whose role in the case of separation of binary mixtures is played by the ideal cascade. As a result, the only universal search method for optimal parameters of the separation cascade is their numerical optimization by the criterion of the minimum number of separation elements in it.

Large gamma-ray detector arrays and electromagnetic separators

NASA Astrophysics Data System (ADS)

Lee, I.-Yang

2013-12-01

The use of large gamma-ray detector arrays with electromagnetic separators is a powerful combination. Various types of gamma-ray detectors have been used; some provide high detector efficiency such as scintillation detector array, others use Ge detectors for good energy resolution, and recently developed Ge energy tracking arrays gives both high peak-to-background ratio and position resolution. Similarly, different types of separators were used to optimize the performance under different experimental requirements and conditions. For example, gas-filled separators were used in heavy element studies for their large efficiency and beam rejection factor. Vacuum separators with good isotope resolution were used in transfer and fragmentation reactions for the study of nuclei far from stability. This paper presents results from recent experiments using gamma-ray detector arrays in combination with electromagnetic separators, and discusses the physics opportunities provided by these instruments. In particular, we review the performance of the instruments currently in use, and discuss the requirements of instruments for future radioactive beam accelerator facilities.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jandel, M.; Bredeweg, T. A.; Fowler, M. M.

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 themore » 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.« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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 themore » 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.« less

(n,{gamma}) Experiments on tin isotopes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baramsai, B.; Mitchell, G. E.; Walker, C. L.

2013-04-19

Neutron capture experiments on highly enriched {sup 117,119}Sn isotopes were performed with the DANCE detector array located at the Los Alamos Neutron Science Center. The DANCE detector provides detailed information about the multi-step {gamma}-ray cascade following neutron capture. Analysis of the experimental data provides important information to improve understanding of the neutron capture reaction, including a test of the statistical model, the assignment of spins and parities of neutron resonances, and information concerning the Photon Strength Function (PSF) and Level Density (LD) below the neutron separation energy. Preliminary results for the (n,{gamma}) reaction on {sup 117,119}Sn are presented. Resonance spinsmore » of the odd-A tin isotopes were almost completely unknown. Resonance spins and parities have been assigned via analysis of the multi-step {gamma}-ray spectra and directional correlations.« less

Nitrogen isotopic analyses by isotope-ratio-monitoring gas chromatography/mass spectrometry

NASA Technical Reports Server (NTRS)

Merritt, D. A.; Hayes, J. M.

1994-01-01

Amino acids containing natural-abundance levels of 15N were derivatized and analyzed isotopically using a technique in which individual compounds are separated by gas chromatography, combusted on-line, and the product stream sent directly to an isotope-ratio mass spectrometer. For samples of N2 gas, standard deviations of ratio measurement were better than 0.1% (Units for delta are parts per thousand or per million (%).) for samples larger than 400 pmol and better than 0.5% for samples larger than 25 pmol (0.1% 15N is equivalent to 0.00004 atom % 15N). Results duplicated those of conventional, batchwise analyses to within 0.05%. For combustion of organic compounds yielding CO2/N2 ratios between 14 and 28, in particular for N-acetyl n-propyl derivatives of amino acids, delta values were within 0.25% of results obtained using conventional techniques and standard deviations were better than 0.35%. Pooled data for measurements of all amino acids produced an accuracy and precision of 0.04 and 0.23%, respectively, when 2 nmol of each amino acid was injected on column and 20% of the stream of combustion products was delivered to the mass spectrometer.

Mixed-mode chromatography/isotope ratio mass spectrometry.

PubMed

McCullagh, James S O

2010-03-15

Liquid chromatography coupled to molecular mass spectrometry (LC/MS) has been a standard technique since the early 1970s but liquid chromatography coupled to high-precision isotope ratio mass spectrometry (LC/IRMS) has only been available commercially since 2004. This development has, for the first time, enabled natural abundance and low enrichment delta(13)C measurements to be applied to individual analytes in aqueous mixtures creating new opportunities for IRMS applications, particularly for the isotopic study of biological molecules. A growing number of applications have been published in a range of areas including amino acid metabolism, carbohydrates studies, quantification of cellular and plasma metabolites, dietary tracer and nucleic acid studies. There is strong potential to extend these to new compounds and complex matrices but several challenges face the development of LC/IRMS methods. To achieve accurate isotopic measurements, HPLC separations must provide baseline-resolution between analyte peaks; however, the design of current liquid interfaces places severe restrictions on compatible flow rates and in particular mobile phase compositions. These create a significant challenge on which reports associated with LC/IRMS have not previously focused. Accordingly, this paper will address aspects of chromatography in the context of LC/IRMS, in particular focusing on mixed-mode separations and their benefits in light of these restrictions. It aims to provide an overview of mixed-mode stationary phases and of ways to improve high aqueous separations through manipulation of parameters such as column length, temperature and mobile phase pH. The results of several practical experiments are given using proteogenic amino acids and nucleosides both of which are of noted importance in the LC/IRMS literature. This communication aims to demonstrate that mixed-mode stationary phases provide a flexible approach given the constraints of LC/IRMS interface design and acts as a

Boron isotope fractionation in liquid chromatography with boron-specific resins as column packing material

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oi, Takao; Shimazaki, Hiromi; Ishii, Reiko

1997-07-01

Boron-specific resins with n-methyl glucamine as the functional group were used as column packing material of liquid chromatography for boron isotope separation. The shapes of chromatograms in reverse breakthrough experiments were heavily dependent on the pH of the eluents, and there existed a pH value at which a chromatogram of the displacement type was realized nearly ideally. The value of the single-stage separation factor for the boron isotopes varied between 1.010 and 1.022, depending on the temperature and the form of the resins. The existence of the three-coordinate boron species in addition to the four-coordinate species in the resin phasemore » is suggested.« less

Molybdenum isotopic evidence for the origin of chondrules and a distinct genetic heritage of carbonaceous and non-carbonaceous meteorites

NASA Astrophysics Data System (ADS)

Budde, Gerrit; Burkhardt, Christoph; Brennecka, Gregory A.; Fischer-Gödde, Mario; Kruijer, Thomas S.; Kleine, Thorsten

2016-11-01

Nucleosynthetic isotope anomalies are powerful tracers to determine the provenance of meteorites and their components, and to identify genetic links between these materials. Here we show that chondrules and matrix separated from the Allende CV3 chondrite have complementary nucleosynthetic Mo isotope anomalies. These anomalies result from the enrichment of a presolar carrier enriched in s-process Mo into the matrix, and the corresponding depletion of this carrier in the chondrules. This carrier most likely is a metal and so the uneven distribution of presolar material probably results from metal-silicate fractionation during chondrule formation. The Mo isotope anomalies correlate with those reported for W isotopes on the same samples in an earlier study, suggesting that the isotope variations for both Mo and W are caused by the heterogeneous distribution of the same carrier. The isotopic complementary of chondrules and matrix indicates that both components are genetically linked and formed together from one common reservoir of solar nebula dust. As such, the isotopic data require that most chondrules formed in the solar nebula and are not a product of protoplanetary impacts. Allende chondrules and matrix together with bulk carbonaceous chondrites and some iron meteorites (groups IID, IIIF, and IVB) show uniform excesses in 92Mo, 95Mo, and 97Mo that result from the addition of supernova material to the solar nebula region in which these carbonaceous meteorites formed. Non-carbonaceous meteorites (enstatite and ordinary chondrites as well as most iron meteorites) do not contain this material, demonstrating that two distinct Mo isotope reservoirs co-existed in the early solar nebula that remained spatially separated for several million years. This separation was most likely achieved through the formation of the gas giants, which cleared the disk between the inner and outer solar system regions parental to the non-carbonaceous and carbonaceous meteorites. The Mo isotope

In-Vivo Zinc Metabolism by Isotope Ratio Mass Spectrometry

USDA-ARS?s Scientific Manuscript database

The purpose of this chapter is to highlight some of the methodological and technical issues surrounding the in vivo use of stable isotopes and to provide examples of how such studies have advanced our knowledge of human zinc metabolism. The advantages and disadvantages of the currently available in...

Detecting intraannual dietary variability in wild mountain gorillas by stable isotope analysis of feces

PubMed Central

Blumenthal, Scott A.; Chritz, Kendra L.; Rothman, Jessica M.; Cerling, Thure E.

2012-01-01

We use stable isotope ratios in feces of wild mountain gorillas (Gorilla beringei) to test the hypothesis that diet shifts within a single year, as measured by dry mass intake, can be recovered. Isotopic separation of staple foods indicates that intraannual changes in the isotopic composition of feces reflect shifts in diet. Fruits are isotopically distinct compared with other staple foods, and peaks in fecal δ13C values are interpreted as periods of increased fruit feeding. Bayesian mixing model results demonstrate that, although the timing of these diet shifts match observational data, the modeled increase in proportional fruit feeding does not capture the full shift. Variation in the isotopic and nutritional composition of gorilla foods is largely independent, highlighting the difficulty for estimating nutritional intake with stable isotopes. Our results demonstrate the potential value of fecal sampling for quantifying short-term, intraindividual dietary variability in primates and other animals with high temporal resolution even when the diet is composed of C3 plants. PMID:23236160

Nd and Sm isotopic composition of spent nuclear fuels from three material test reactors

DOE PAGES

Sharp, Nicholas; Ticknor, Brian W.; Bronikowski, Michael; ...

2016-11-17

Rare earth elements such as neodymium and samarium are ideal for probing the neutron environment that spent nuclear fuels are exposed to in nuclear reactors. The large number of stable isotopes can provide distinct isotopic signatures for differentiating the source material for nuclear forensic investigations. The rare-earth elements were isolated from the high activity fuel matrix via ion exchange chromatography in a shielded cell. The individual elements were then separated using cation exchange chromatography. In conclusion, the neodymium and samarium aliquots were analyzed via MC–ICP–MS, resulting in isotopic compositions with a precision of 0.01–0.3%.

Nd and Sm isotopic composition of spent nuclear fuels from three material test reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sharp, Nicholas; Ticknor, Brian W.; Bronikowski, Michael

Rare earth elements such as neodymium and samarium are ideal for probing the neutron environment that spent nuclear fuels are exposed to in nuclear reactors. The large number of stable isotopes can provide distinct isotopic signatures for differentiating the source material for nuclear forensic investigations. The rare-earth elements were isolated from the high activity fuel matrix via ion exchange chromatography in a shielded cell. The individual elements were then separated using cation exchange chromatography. In conclusion, the neodymium and samarium aliquots were analyzed via MC–ICP–MS, resulting in isotopic compositions with a precision of 0.01–0.3%.

A Guide for Assessing Biodegradation and Source Identification of Organic Groundwater Contaminants Using Compound Specific Isotope Analysis (CSIA)

EPA Science Inventory

When organic contaminants are degraded in the environment, the ratio of stable isotopes will often change, and the extent of degradation can be recognized and predicted from the change in the ratio of stable isotopes. Recent advances in analytical chemistry make it possible to p...

Separation of Pb, Bi and Po by cation exchange resin

DOE PAGES

Kmak, Kelly N.; Despotopulos, John D.; Shaughnessy, Dawn A.

2017-09-27

In this paper, a separation of 209Po, 207Bi and 212Pb using AG 50Wx8 and AG MP 50 cation exchange resins in an HCl medium was developed. A procedure in which Po(IV) elutes first in 0.2 M HCl, followed by Bi(III) in 0.4 M HCl and finally Pb(II) in 2 M HCl was established. The separation using AG 50Wx8 provides a much better elution profile than that of AG MP 50 with no overlap between the elution bands. Finally, this separation has the potential to be used as an isotope generator for producing 210Po from 210Pb.

Kinetic isotopic fractionation during diffusion of ionic species in water

NASA Astrophysics Data System (ADS)

Richter, Frank M.; Mendybaev, Ruslan A.; Christensen, John N.; Hutcheon, Ian D.; Williams, Ross W.; Sturchio, Neil C.; Beloso, Abelardo D.

2006-01-01

Experiments specifically designed to measure the ratio of the diffusivities of ions dissolved in water were used to determine DLi/DK,D/D,D/D,D/D,andD/D. The measured ratio of the diffusion coefficients for Li and K in water (D Li/D K = 0.6) is in good agreement with published data, providing evidence that the experimental design being used resolves the relative mobility of ions with adequate precision to also be used for determining the fractionation of isotopes by diffusion in water. In the case of Li, we found measurable isotopic fractionation associated with the diffusion of dissolved LiCl (D/D=0.99772±0.00026). This difference in the diffusion coefficient of 7Li compared to 6Li is significantly less than that reported in an earlier study, a difference we attribute to the fact that in the earlier study Li diffused through a membrane separating the water reservoirs. Our experiments involving Mg diffusing in water found no measurable isotopic fractionation (D/D=1.00003±0.00006). Cl isotopes were fractionated during diffusion in water (D/D=0.99857±0.00080) whether or not the co-diffuser (Li or Mg) was isotopically fractionated. The isotopic fractionation associated with the diffusion of ions in water is much smaller than values we found previously for the isotopic fractionation of Li and Ca isotopes by diffusion in molten silicate liquids. A major distinction between water and silicate liquids is that water surrounds dissolved ions with hydration shells, which very likely play an important but still poorly understood role in limiting the isotopic fractionation associated with diffusion.

An improved procedure for separation/purification of boron from complex matrices and high-precision measurement of boron isotopes by positive thermal ionization and multicollector inductively coupled plasma mass spectrometry.

PubMed

Wei, Hai-Zhen; Jiang, Shao-Yong; Hemming, N Gary; Yang, Jing-Hong; Yang, Tao; Wu, He-Pin; Yang, Tang-Li; Yan, Xiong; Pu, Wei

2014-06-01

In order to eliminate boron loss and potential isotopic fractionation during chemical pretreatment of natural samples with complex matrices, a three-column ion-exchange separation/purification procedure has been modified, which ensures more than 98% recovery of boron from each step for a wide range of sample matrices, and is applicable for boron isotope analysis by both TIMS and MC-ICP-MS. The PTIMS-Cs2BO2(+)-static double collection method was developed, ensuring simultaneous collection of (133)Cs2(11)B(16)O2(+)(m/z 309) and (133)Cs2(10)B(16)O2(+) (m/z 308) ions in adjacent H3-H4 Faraday cups with typical zoom optics parameters (Focus Quad: 15 V, Dispersion Quad: -85 V). The external reproducibilities of the measured (11)B/(10)B ratios of the NIST 951 boron standard solutions of 1000 ng, 100 ng and 10 ng of boron by PTIMS method are ±0.06‰, ±0.16‰ and ±0.25‰, respectively, which indicates excellent precision can be achieved for boron isotope measurement at nanogram level boron in natural samples. An on-peak zero blank correction procedure was employed to correct the residual boron signals effect in MC-ICP-MS, which gives consistent δ(11)B values with a mean of 39.66±0.35‰ for seawater in the whole range of boron content from 5 ppb to 200 ppb, ensuring accurate boron isotope analysis in few ppb boron. With the improved protocol, consistent results between TIMS and MC-ICP-MS data were obtained in typical geological materials within a wide span of δ(11)B values ranging from -25‰ to +40‰. Copyright © 2014 Elsevier B.V. All rights reserved.

Separation of malignant human breast cancer epithelial cells from healthy epithelial cells using an advanced dielectrophoresis-activated cell sorter (DACS).

PubMed

An, Jaemin; Lee, Jangwon; Lee, Sang Ho; Park, Jungyul; Kim, Byungkyu

2009-06-01

In this paper, we successfully separated malignant human breast cancer epithelial cells (MCF 7) from healthy breast cells (MCF 10A) and analyzed the main parameters that influence the separation efficiency with an advanced dielectrophoresis (DEP)-activated cell sorter (DACS). Using the efficient DACS, the malignant cancer cells (MCF 7) were isolated successfully by noninvasive methods from normal cells with similar cell size distributions (MCF 10A), depending on differences between their material properties such as conductivity and permittivity, because our system was able to discern the subtle differences in the properties by generating continuously changed electrical field gradients. In order to evaluate the separation performance without considering size variations, the cells collected from each outlet were divided into size-dependent groups and counted statistically. Following that, the quantitative relative ratio of numbers between MCF 7 and MCF 10A cells in each size-dependent group separated by the DEP were compared according to applied frequencies in the range 48, 51, and 53 MHz with an applied amplitude of 8 V(pp). Finally, under the applied voltage of 48 MHz-8 V(pp) and a flow rate of 290 microm/s, MCF 7 and MCF 10A cells were separated with a maximum efficiency of 86.67% and 98.73% respectively. Therefore, our suggested system shows it can be used for detection and separation of cancerous epithelial cells from noncancerous cells in clinical applications.

Inorganic separator technology program

NASA Technical Reports Server (NTRS)

Smatko, J. S.; Weaver, R. D.; Kalhammer, F. R.

1973-01-01

Testing and failure analyses of silver zinc cells with largely inorganic separators were performed. The results showed that the wet stand and cycle life objective of the silver-zinc cell development program were essentially accomplished and led to recommendations for cell composition, design, and operation that should yield further improvement in wet and cycle life. A series of advanced inorganic materials was successfully developed and formulated into rigid and semiflexible separator samples. Suitable screening tests for evaluation of largely inorganic separators were selected and modified for application to the separator materials. The results showed that many of these formulations are potentially superior to previously used materials and permitted selection of three promising materials for further evaluation in silver-zinc cells.

Stable isotopes and elasmobranchs: tissue types, methods, applications and assumptions.

PubMed

Hussey, N E; MacNeil, M A; Olin, J A; McMeans, B C; Kinney, M J; Chapman, D D; Fisk, A T

2012-04-01

Stable-isotope analysis (SIA) can act as a powerful ecological tracer with which to examine diet, trophic position and movement, as well as more complex questions pertaining to community dynamics and feeding strategies or behaviour among aquatic organisms. With major advances in the understanding of the methodological approaches and assumptions of SIA through dedicated experimental work in the broader literature coupled with the inherent difficulty of studying typically large, highly mobile marine predators, SIA is increasingly being used to investigate the ecology of elasmobranchs (sharks, skates and rays). Here, the current state of SIA in elasmobranchs is reviewed, focusing on available tissues for analysis, methodological issues relating to the effects of lipid extraction and urea, the experimental dynamics of isotopic incorporation, diet-tissue discrimination factors, estimating trophic position, diet and mixing models and individual specialization and niche-width analyses. These areas are discussed in terms of assumptions made when applying SIA to the study of elasmobranch ecology and the requirement that investigators standardize analytical approaches. Recommendations are made for future SIA experimental work that would improve understanding of stable-isotope dynamics and advance their application in the study of sharks, skates and rays. © 2012 The Authors. Journal of Fish Biology © 2012 The Fisheries Society of the British Isles.

Testing sequential extraction methods for the analysis of multiple stable isotope systems from a bone sample

NASA Astrophysics Data System (ADS)

Sahlstedt, Elina; Arppe, Laura

2017-04-01

Stable isotope composition of bones, analysed either from the mineral phase (hydroxyapatite) or from the organic phase (mainly collagen) carry important climatological and ecological information and are therefore widely used in paleontological and archaeological research. For the analysis of the stable isotope compositions, both of the phases, hydroxyapatite and collagen, have their more or less well established separation and analytical techniques. Recent development in IRMS and wet chemical extraction methods have facilitated the analysis of very small bone fractions (500 μg or less starting material) for PO43-O isotope composition. However, the uniqueness and (pre-) historical value of each archaeological and paleontological finding lead to preciously little material available for stable isotope analyses, encouraging further development of microanalytical methods for the use of stable isotope analyses. Here we present the first results in developing extraction methods for combining collagen C- and N-isotope analyses to PO43-O-isotope analyses from a single bone sample fraction. We tested sequential extraction starting with dilute acid demineralization and collection of both collagen and PO43-fractions, followed by further purification step by H2O2 (PO43-fraction). First results show that bone sample separates as small as 2 mg may be analysed for their δ15N, δ13C and δ18OPO4 values. The method may be incorporated in detailed investigation of sequentially developing skeletal material such as teeth, potentially allowing for the investigation of interannual variability in climatological/environmental signals or investigation of the early life history of an individual.

Advanced coal cleaning meets acid rain emission limits

DOE Office of Scientific and Technical Information (OSTI.GOV)

Boron, D.J.; Matoney, J.P.; Albrecht, M.C.

1987-03-01

The following processes were selected for study: fine-coal, heavy-medium cyclone separation/flotation, advanced flotation, Dow true heavy liquid separation, Advanced Energy Dynamics (AED) electrostatic separation, and National Research Council of Canada oil agglomeration. Advanced coal cleaning technology was done for the state of New York to investigate methods to use high sulfur coal in view of anticipated lower SO/sub 2/ emission limits.

Trophic spectra under the lens of amino acid isotopic analysis

USDA-ARS?s Scientific Manuscript database

Recent advances in compound specific isotopic ratio analysis (CSIRA) have allowed researchers to measure trophic fractionation of 15N in specific amino acids, namely glutamic acid and phenylalanine. These amino acids have proven useful in food web studies because of the wide and consistent disparity...

Isotopic decoupling during porous melt flow: A case-study in the Lherz peridotite

NASA Astrophysics Data System (ADS)

Le Roux, V.; Bodinier, J.-L.; Alard, O.; O'Reilly, S. Y.; Griffin, W. L.

2009-03-01

Most peridotite massifs and mantle xenoliths show a wide range of isotopic variations, often involving significant decoupling between Hf, Nd and Sr isotopes. These variations are generally ascribed either to mingling of individual components of contrasted isotopic compositions or to time integration of parent-element enrichment by percolating melts/fluids, superimposed onto previous depletion event(s). However, strong isotopic decoupling may also arise during porous flow as a result of daughter-elements fractionation during solid-liquid interaction. Although porous flow is recognized as an important process in mantle rocks, its effects on mantle isotopic variability have been barely investigated so far. The peridotites of the Lherz massif (French Pyrenees) display a frozen melt percolation front separating highly refractory harzburgites from refertilized lherzolites. Isotopic signatures observed at the melt percolation front show a strong decoupling of Hf from Nd and Sr isotopes that cannot be accounted for by simple mixing involving the harzburgite protolith and the percolating melt. Using one dimensional percolation-diffusion and percolation-reaction modeling, we show that these signatures represent transient isotopic compositions generated by porous flow. These signatures are governed by a few critical parameters such as daughter element concentrations in melt and peridotite, element diffusivity, and efficiency of isotopic homogenization rather than by the chromatographic effect of melt transport and the refertilization reaction. Subtle variations in these parameters may generate significant inter-isotopic decoupling and wide isotopic variations in mantle rocks.

Recent advances in liquid-phase separations for clinical metabolomics.

PubMed

Kohler, Isabelle; Giera, Martin

2017-01-01

Over the last decades, several technological improvements have been achieved in liquid-based separation techniques, notably, with the advent of fully porous sub-2 μm particles and superficially porous sub-3 μm particles, the comeback of supercritical fluid chromatography, and the development of alternative chromatographic modes such as hydrophilic interaction chromatography. Combined with mass spectrometry, these techniques have demonstrated their added value, substantially increasing separation efficiency, selectivity, and speed of analysis. These benefits are essential in modern clinical metabolomics typically involving the study of large-scale sample cohorts and the analysis of thousands of metabolites showing extensive differences in physicochemical properties. This review presents a brief overview of the recent developments in liquid-phase separation sciences in the context of clinical metabolomics, focusing on increased throughput as well as metabolite coverage. Relevant metabolomics applications highlighting the benefits of ultra-high performance liquid chromatography, core-shell technology, high-temperature liquid chromatography, capillary electrophoresis, supercritical fluid chromatography, and hydrophilic interaction chromatography are discussed. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Biometrics from the carbon isotope ratio analysis of amino acids in human hair.

PubMed

Jackson, Glen P; An, Yan; Konstantynova, Kateryna I; Rashaid, Ayat H B

2015-01-01

This study compares and contrasts the ability to classify individuals into different grouping factors through either bulk isotope ratio analysis or amino-acid-specific isotope ratio analysis of human hair. Using LC-IRMS, we measured the isotope ratios of 14 amino acids in hair proteins independently, and leucine/isoleucine as a co-eluting pair, to provide 15 variables for classification. Multivariate analysis confirmed that the essential amino acids and non-essential amino acids were mostly independent variables in the classification rules, thereby enabling the separation of dietary factors of isotope intake from intrinsic or phenotypic factors of isotope fractionation. Multivariate analysis revealed at least two potential sources of non-dietary factors influencing the carbon isotope ratio values of the amino acids in human hair: body mass index (BMI) and age. These results provide evidence that compound-specific isotope ratio analysis has the potential to go beyond region-of-origin or geospatial movements of individuals-obtainable through bulk isotope measurements-to the provision of physical and characteristic traits about the individuals, such as age and BMI. Further development and refinement, for example to genetic, metabolic, disease and hormonal factors could ultimately be of great assistance in forensic and clinical casework. Copyright © 2014 Forensic Science Society. Published by Elsevier Ireland Ltd. All rights reserved.

A Review of State-of-the-Art Separator Materials for Advanced Lithium-Based Batteries for Future Aerospace Missions

NASA Technical Reports Server (NTRS)

Bladwin, Richard S.

2009-01-01

As NASA embarks on a renewed human presence in space, safe, human-rated, electrical energy storage and power generation technologies, which will be capable of demonstrating reliable performance in a variety of unique mission environments, will be required. To address the future performance and safety requirements for the energy storage technologies that will enhance and enable future NASA Constellation Program elements and other future aerospace missions, advanced rechargeable, lithium-ion battery technology development is being pursued with an emphasis on addressing performance technology gaps between state-of-the-art capabilities and critical future mission requirements. The material attributes and related performance of a lithium-ion cell's internal separator component are critical for achieving overall optimal performance, safety and reliability. This review provides an overview of the general types, material properties and the performance and safety characteristics of current separator materials employed in lithium-ion batteries, such as those materials that are being assessed and developed for future aerospace missions.

Evaluating Snowmelt Runoff Processes Using Stable Isotopes in a Permafrost Hillslope

NASA Astrophysics Data System (ADS)

Carey, S. K.

2004-05-01

Conceptual understanding of runoff generation in permafrost regions have been derived primarily from hydrometric information, with isotope and hydrochemical data having only limited application in delineating sources and pathways of water. Furthermore, when stable isotope data are used to infer runoff processes, it often provides conflicting results from hydrometric measurements. In a small subarctic alpine catchment within the Wolf Creek Research Basin, Yukon, Canada, experiments were conducted during the melt period of 2002 and 2003 to trace the stable isotopic signature (d18O) of meltwater from a melting snowpack into permafrost soils and laterally to the stream to identify runoff processes and evaluate sources of error for traditional hydrograph separation studies in snowmelt-dominated permafrost basins. Isotopic variability in the snowpack was recorded at 0.1 m depth intervals during the melt period and compared with the meltwater isotopic signature at the snowpack base collected in lysimeters. Throughout the melt period in both years, there was an isotopic enrichment of meltwater as the season progressed. A downslope transect of wells and piezometers were used to evaluate the influence of infiltrating meltwater and thawing ground on the subsurface d18O signature. As melt began, meltwater infiltrated the frozen porous organic layer, leading to liquid water saturation in the unsaturated pore spaces. Water sampled during this initial melt stage show soil water d18O mirroring that of the meltwater signal. As the melt season progressed, frozen soil began to melt, mixing enriched pre-melt soil water with meltwater. This mixing increased the overall value of d18O obtained from the soil, which gradually increased as thaw progressed. At the end of snowmelt, soil water had a d18O value similar to values from the previous fall, suggesting that much of the initial snowmelt water had been flushed from the hillslope. Results from the hillslope scale are compared with two

Copper isotope fractionation during surface adsorption and intracellular incorporation by bacteria

PubMed Central

Navarrete, Jesica U.; Borrok, David M.; Viveros, Marian; Ellzey, Joanne T.

2011-01-01

Copper isotopes may prove to be a useful tool for investigating bacteria–metal interactions recorded in natural waters, soils, and rocks. However, experimental data which attempt to constrain Cu isotope fractionation in biologic systems are limited and unclear. In this study, we utilized Cu isotopes (δ65Cu) to investigate Cu–bacteria interactions, including surface adsorption and intracellular incorporation. Experiments were conducted with individual representative species of Gram-positive (Bacillus subtilis) and Gram-negative (Escherichia coli) bacteria, as well as with wild-type consortia of microorganisms from several natural environments. Ph-dependent adsorption experiments were conducted with live and dead cells over the pH range 2.5–6. Surface adsorption experiments of Cu onto live bacterial cells resulted in apparent separation factors (Δ65Cusolution–solid = δ65Cusolution – δ65Cusolid) ranging from +0.3‰ to +1.4‰ for B. subtilis and +0.2‰ to +2.6‰ for E. coli. However, because heat-killed bacterial cells did not exhibit this behavior, the preference of the lighter Cu isotope by the cells is probably not related to reversible surface adsorption, but instead is a metabolically-driven phenomenon. Adsorption experiments with heat-killed cells yielded apparent separation factors ranging from +0.3‰ to –0.69‰ which likely reflects fractionation from complexation with organic acid surface functional group sites. For intracellular incorporation experiments the lab strains and natural consortia preferentially incorporated the lighter Cu isotope with an apparent Δ65Cusolution–solid ranging from ~+1.0‰ to +4.4‰. Our results indicate that live bacterial cells preferentially sequester the lighter Cu isotope regardless of the experimental conditions. The fractionation mechanisms involved are likely related to active cellular transport and regulation, including the reduction of Cu(II) to Cu(I). Because similar intracellular Cu machinery is

VAPOR PRESSURE ISOTOPE EFFECTS IN THE MEASUREMENT OF ENVIRONMENTAL TRITIUM SAMPLES.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuhne, W.

2012-12-03

Standard procedures for the measurement of tritium in water samples often require distillation of an appropriate sample aliquot. This distillation process may result in a fractionation of tritiated water and regular light water due to the vapor pressure isotope effect, introducing either a bias or an additional contribution to the total tritium measurement uncertainty. The magnitude of the vapor pressure isotope effect is characterized as functions of the amount of water distilled from the sample aliquot and the heat settings for the distillation process. The tritium concentration in the distillate is higher than the tritium concentration in the sample earlymore » in the distillation process, it then sharply decreases due to the vapor pressure isotope effect and becomes lower than the tritium concentration in the sample, until the high tritium concentration retained in the boiling flask is evaporated at the end of the process. At that time, the tritium concentration in the distillate again overestimates the sample tritium concentration. The vapor pressure isotope effect is more pronounced the slower the evaporation and distillation process is conducted; a lower heat setting during the evaporation of the sample results in a larger bias in the tritium measurement. The experimental setup used and the fact that the current study allowed for an investigation of the relative change in vapor pressure isotope effect in the course of the distillation process distinguish it from and extend previously published measurements. The separation factor as a quantitative measure of the vapor pressure isotope effect is found to assume values of 1.034 {+-} 0.033, 1.052 {+-} 0.025, and 1.066 {+-} 0.037, depending on the vigor of the boiling process during distillation of the sample. A lower heat setting in the experimental setup, and therefore a less vigorous boiling process, results in a larger value for the separation factor. For a tritium measurement in water samples, this implies

[Advancements of computer chemistry in separation of Chinese medicine].

PubMed

Li, Lingjuan; Hong, Hong; Xu, Xuesong; Guo, Liwei

2011-12-01

Separating technique of Chinese medicine is not only a key technique in the field of Chinese medicine' s research and development, but also a significant step in the modernization of Chinese medicinal preparation. Computer chemistry can build model and look for the regulations from Chinese medicine system which is full of complicated data. This paper analyzed the applicability, key technology, basic mode and common algorithm of computer chemistry applied in the separation of Chinese medicine, introduced the mathematic mode and the setting methods of Extraction kinetics, investigated several problems which based on traditional Chinese medicine membrane procession, and forecasted the application prospect.

Paleoclimate and Amerindians: Evidence from stable isotopes and atmospheric circulation

USGS Publications Warehouse

Lovvorn, M.B.; Frison, G.C.; Tieszen, L.L.

2001-01-01

Two Amerindian demographic shifts are attributed to climate change in the northwest plains of North America: at ???11,000 calendar years before present (yr BP), Amerindian culture apparently split into foothills-mountains vs. plains biomes; and from 8,000-5,000 yr BP, scarce archaeological sites on the open plains suggest emigration during xeric "Altithermal" conditions. We reconstructed paleoclimates from stable isotopes in prehistoric bison bone and relations between weather and fractions of C4 plants in forage. Further, we developed a climate-change model that synthesized stable isotope, existing qualitative evidence (e.g., palynological, erosional), and global climate mechanisms affecting this midlatitude region. Our isotope data indicate significant warming from ???12,400 to 11,900 yr BP, supporting climate-driven cultural separation. However, isotope evidence of apparently wet, warm conditions at 7,300 yr BP refutes emigration to avoid xeric conditions. Scarcity of archaeological sites is best explained by rapid climate fluctuations after catastrophic draining of the Laurentide Lakes, which disrupted North Atlantic Deep Water production and subsequently altered monsoonal inputs to the open plains.

Tooth enamel maturation reequilibrates oxygen isotope compositions and supports simple sampling methods

NASA Astrophysics Data System (ADS)

Trayler, Robin B.; Kohn, Matthew J.

2017-02-01

Oxygen isotope and major element zoning patterns of several disparate ungulate teeth were collected to evaluate the timing and geometry of enamel formation, records of isotope zoning, and tooth enamel sampling strategies. Isotopic zoning in mammalian tooth enamel encodes a sub-annual time series of isotopic variation of an animal's body water composition, with a damping factor that depends on the specifics of how enamel mineralizes. Enamel formation comprises two stages: precipitation of appositional enamel with a high CO3:PO4 ratio, followed by precipitation of maturational enamel with a lower CO3:PO4. If appositional and maturational enamel both contribute to isotope compositions (but with different CO3:PO4), and if isotope compositions vary seasonally, paired δ18O values from CO3 and PO4 profiles should show a spatial separation. CO3 isotope patterns should be shifted earlier seasonally than PO4 isotope patterns. Such paired profiles for new and published data show no resolvable shifts, i.e. CO3 and PO4 δ18O profiles show coincident maxima and minima. This coincidence suggests that enamel maturation reequilibrates appositional isotope compositions. If enamel maturation establishes enamel isotope compositions, the geometry of maturation, not apposition, should be considered when devising sampling protocols. X-ray maps of Ca zoning show that the majority of enamel (inner and middle layers) mineralizes heavily at a high angle to the external tooth surface and the enamel-dentine junction over length scales of 2-4 mm, while the outer enamel surface mineralizes more slowly. These data suggest that isotopic sampling strategies should parallel maturational geometry and focus on interior enamel to improve data fidelity. The magnitude of isotopic damping is also smaller than implied in previous studies, so tooth enamel zoning more closely reflects original body water isotopic variations than previously assumed.

Liquid and gas chromatography coupled to isotope ratio mass spectrometry for the determination of 13C-valine isotopic ratios in complex biological samples.

PubMed

Godin, Jean-Philippe; Breuillé, Denis; Obled, Christiane; Papet, Isabelle; Schierbeek, Henk; Hopfgartner, Gérard; Fay, Laurent-Bernard

2008-10-01

On-line gas chromatography-combustion-isotope ratio mass spectrometry (GC-C-IRMS) is commonly used to measure isotopic ratios at natural abundance as well as for tracer studies in nutritional and medical research. However, high-precision (13)C isotopic enrichment can also be measured by liquid chromatography-isotope ratio mass spectrometry (LC-IRMS). Indeed, LC-IRMS can be used, as shown by the new method reported here, to obtain a baseline separation and to measure (13)C isotopic enrichment of underivatised amino acids (Asp, Thr-Ser, Glu, Pro, Gly, Ala, Cys and Val). In case of Val, at natural abundance, the SD(delta(13)C) reported with this method was found to be below 1 per thousand . Another key feature of the new LC-IRMS method reported in this paper is the comparison of the LC-IRMS approach with the conventional GC-C-IRMS determination. To perform this comparative study, isotopic enrichments were measured from underivatised Val and its N(O, S)-ethoxycarbonyl ethyl ester derivative. Between 0.0 and 1.0 molar percent excess (MPE) (delta(13)C= -12.3 to 150.8 per thousand), the calculated root-mean-square (rms) of SD was 0.38 and 0.46 per thousand and the calculated rms of accuracy was 0.023 and 0.005 MPE, respectively, for GC-C-IRMS and LC-IRMS. Both systems measured accurately low isotopic enrichments (0.002 atom percent excess (APE)) with an SD (APE) of 0.0004. To correlate the relative (delta(13)C) and absolute (atom%, APE and MPE) isotopic enrichment of Val measured by the GC-C-IRMS and LC-IRMS devices, mathematical equations showing the slope and intercept of the curves were established and validated with experimental data between 0.0 to 2.3 MPE. Finally, both GC-C-IRMS and LC-IRMS instruments were also used to assess isotopic enrichment of protein-bound (13)C-Val in tibial epiphysis in a tracer study performed in rats. Isotopic enrichments measured by LC-IRMS and GC-C-IRMS were not statistically different (p>0.05). The results of this work indicate that

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.

Measurements of Forest-Atmosphere Isotopic CO2 Exchange by Eddy Covariance

NASA Astrophysics Data System (ADS)

Wehr, R. A.; Munger, J. W.; Nelson, D. D.; McManus, J. B.; Zahniser, M. S.; Saleska, S. R.

2010-12-01

Isotopic CO2 flux measurements are a promising means for partitioning the net ecosystem exchange of CO2 into photosynthetic and respiratory components. This approach to partitioning is possible in principle because of the distinct isotopic signatures of respired and photosynthesized CO2, but has been infeasible in practice—especially in forests—because of the difficulty of measuring isotopic ratios with sufficient precision and time response for use in eddy covariance (EC) flux calculations. Recent advances in laser spectroscopic instrumentation have changed that. We report measurements of isotopic (13C and 18O) CO2 exchange made by eddy covariance at Harvard Forest between April and December, 2010. The measurements were made using a continuous-wave quantum cascade laser spectrometer (Aerodyne Research Inc.) sampling at 4 Hz and are, to our knowledge, the first EC isotopic flux measurements at a forest site. The spectrometer can measure δ13C and δ18O with internal precisions (standard deviation of 1-minute averages) of 0.03 ‰, and [CO2] with an internal precision of 15 ppb; the instrumental accuracy, calibration, and long-term stability are discussed in detail. The isotopic data are considered in relation to environmental variables (PAR, temperature, humidity, soil temperature and moisture), and a first attempt at flux partitioning using the isotopic fluxes is presented.

Observation of the isotope effect in sub-kelvin reactions

NASA Astrophysics Data System (ADS)

Lavert-Ofir, Etay; Shagam, Yuval; Henson, Alon B.; Gersten, Sasha; Kłos, Jacek; Żuchowski, Piotr S.; Narevicius, Julia; Narevicius, Edvardas

2014-04-01

Quantum phenomena in the translational motion of reactants, which are usually negligible at room temperature, can dominate reaction dynamics at low temperatures. In such cold conditions, even the weak centrifugal force is enough to create a potential barrier that keeps reactants separated. However, reactions may still proceed through tunnelling because, at low temperatures, wave-like properties become important. At certain de Broglie wavelengths, the colliding particles can become trapped in long-lived metastable scattering states, leading to sharp increases in the total reaction rate. Here, we show that these metastable states are responsible for a dramatic, order-of-magnitude-strong, quantum kinetic isotope effect by measuring the absolute Penning ionization reaction rates between hydrogen isotopologues and metastable helium down to 0.01 K. We demonstrate that measurements of a single isotope are insufficient to constrain ab initio calculations, making the kinetic isotope effect in the cold regime necessary to remove ambiguity among possible potential energy surfaces.

Illuminating hydrological processes at the soil-vegetation-atmosphere interface with water stable isotopes

NASA Astrophysics Data System (ADS)

Sprenger, Matthias; Leistert, Hannes; Gimbel, Katharina; Weiler, Markus

2016-09-01

Water stable isotopes (18O and 2H) are widely used as ideal tracers to track water through the soil and to separate evaporation from transpiration. Due to the technical developments in the last two decades, soil water stable isotope data have become easier to collect. Thus, the application of isotope methods in soils is growing rapidly. Studies that make use of soil water stable isotopes often have a multidisciplinary character since an interplay of processes that take place in the vadose zone has to be considered. In this review, we provide an overview of the hydrological processes that alter the soil water stable isotopic composition and present studies utilizing pore water stable isotopes. The processes that are discussed include the water input as precipitation or throughfall, the output as evaporation, transpiration, or recharge, and specific flow and transport processes. Based on the review and supported by additional data and modeling results, we pose a different view on the recently proposed two water world hypothesis. As an alternative to two distinct pools of soil water, where one pool is enriched in heavy isotopes and used by the vegetation and the other pool does not undergo isotopic fractionation and becomes recharge, the water gets successively mixed with newly introduced rainwater during the percolation process. This way, water initially isotopically enriched in the topsoil loses the fractionation signal with increasing infiltration depth, leading to unfractionated isotopic signals in the groundwater.

Spectroscopic Measurement of LEAD-204 Isotope Shift and LEAD-205 Nuclear Spin.

NASA Astrophysics Data System (ADS)

Schonberger, Peter

The isotope shift of ('204)Pb and the nuclear spin of 1.4 x 10('7)-y ('205)Pb was determined from a high -resolution optical measurement of the 6p('2) ('3)P(,o) -6p7s('3)P(,1)('o) 283.3-nm resonance line. The value of the shift, relative to ('208)Pb is -140.2(8) x 10('-3)cm(' -1), the negative sign indicating a shift to lower wave numbers. The precision is 3-4 times greater than that of previous measurements. The spin of ('205)Pb l = 5/2 was obtained from the measurement of the relative intensities of its three hyperfine components. This method of absorption spectroscopy determination of ground state nuclear spin is applicable to any stable or longlived isotope. High resolution optical absorption spectra were obtained with a 25.4cm diffraction grating in a 9.1m focal length Czerny-Turner spectrometer. A signal-averaging scanning technique was used to record the spectra. Increased precision in the isotope shift measurement was attained by using separated isotope samples of ('204)Pb and ('207)Pb. A controlled amount of the later was incorporated in the absorption cell to provide internal calibration by its 6p7s ('3)P(,1)('o) hfs separation. Absorption spectra were recorded for several optical thicknesses of the absorber. A single spin value of increased precision was derived from the entire set of combined data.

Baseflow separation in a premontane transitional rainforest using stable isotope techniques

NASA Astrophysics Data System (ADS)

Miller, G. R.; DuMont, A.; Roark, E.; Cahill, A. T.; Brumbelow, J. K.

2013-12-01

Hydrologic, geologic, and biologic processes are critical to understanding the ecosystem in the tropical premontane transitional forests of Costa Rica. Precipitation is significantly lower during the dry season, and incoming rainfall can be completely intercepted and re-evaporated by the canopy during light events. These canopy processes can affect the rates of runoff and infiltration by changing the quantity and timing of rainfall reaching the ground surface. However, the resulting partitioning of stream water sources between event-water and baseflow from groundwater is not well quantified due to limited accessibility and complex subsurface conditions. This study focuses on research conducted at the Texas A&M Soltis Center for Education and Research, near San Ramón, Costa Rica. We have monitored a 2.2 ha watershed there, measuring precipitation and transpiration rates for over two years, and groundwater levels and stream flow rates for nearly one year. Precipitation rates for the watershed averaged 4.4 m/yr since 2010. Stream flow (runoff, spring flow, and baseflow) averaged 0.09 m^3/sec during the 2012-2013 wet seasons. At 1.2 mm/day, transpiration was a relatively minor component of the water budget. Over a 40-day span during summer 2013, we collected a combination of daily and rain-event based samples from locations throughout the watershed. Sources included: the main stream and two small tributaries, groundwater from piezometers, pore water from suction lysimeters, throughfall and stemflow from under canopy collection systems, and xylem water from 8 tree species across the watershed. We then measured stable isotope fractions (δ18O and δD) in the water using a Picarro L2120i CRDS. Isotope ratios for all surface water averaged -5.50‰ for δ18O and -28.00‰ for δD, while that measured under baseflow conditions were -5.45‰ for δ18O and -29.18‰ for δD. These results indicate that baseflow is the dominate source of stream water even in the wet season

Monitoring steel bridge renovation using lead isotopic tracing.

PubMed

Salome, Fred; Gulson, Brian; Chiaradia, Massimo; Davis, Jeffrey; Morris, Howard

2017-05-01

Monitoring removal of lead (Pb) paint from steel structures usually involves analysis of environmental samples for total lead and determination of blood Pb levels of employees involved in the Pb paint removal. We used high precision Pb isotopic tracing for a bridge undergoing Pb paint removal to determine if Pb in the environmental and blood samples originated from the bridge paint. The paint system on the bridge consisted of an anti-corrosive red Pb primer top-coated with a Micaceous Iron Oxide (MIO) alkyd. Analysis of the red Pb primer gave uniform isotopic ratios indicative of Pb from the geologically-ancient Broken Hill mines in western New South Wales, Australia. Likewise waste abrasive material, as anticipated, had the same isotopic composition as the paint. The isotopic ratios for other samples lay on 2 separate linear arrays on a 207 Pb/ 204 Pb versus 206 Pb/ 204 Pb diagram, one largely defined by gasoline and the majority of the ambient air data, and the other by data for one sample each of gasoline and ambient air and underwater sediments. Isotopic ratios in background ambient air samples for the project were characteristic of leaded gasoline. Air sampling during paint removal showed a contribution of paint Pb ranging from about 20 to 40%. Isotopic ratios in the blood of 8 employees prior to the commencement of work showed that 6 of these had been previously exposed to the Broken Hill Pb possibly from earlier bridge paint removal projects. One subject appeared to have increased exposure to Pb probably from the paint renovations. Copyright © 2017 Elsevier Ltd. All rights reserved.

Equilibrium properties of dense hydrogen isotope gases based on the theory of simple fluids.

PubMed

Kowalczyk, Piotr; MacElroy, J M D

2006-08-03

We present a new method for the prediction of the equilibrium properties of dense gases containing hydrogen isotopes. The proposed approach combines the Feynman-Hibbs effective potential method and a deconvolution scheme introduced by Weeks et al. The resulting equations of state and the chemical potentials as functions of pressure for each of the hydrogen isotope gases depend on a single set of Lennard-Jones parameters. In addition to its simplicity, the proposed method with optimized Lennard-Jones potential parameters accurately describes the equilibrium properties of hydrogen isotope fluids in the regime of moderate temperatures and pressures. The present approach should find applications in the nonlocal density functional theory of inhomogeneous quantum fluids and should also be of particular relevance to hydrogen (clean energy) storage and to the separation of quantum isotopes by novel nanomaterials.

Applications of DNA-Stable Isotope Probing in Bioremediation Studies

NASA Astrophysics Data System (ADS)

Chen, Yin; Vohra, Jyotsna; Murrell, J. Colin

DNA-stable isotope probing, a method to identify active microorganisms without the prerequisite of cultivation, has been widely applied in the study of microorganisms involved in the degradation of environmental pollutants. Recent advances and technique considerations in applying DNA-SIP in bioremediation are highlighted. A detailed protocol of a DNA-SIP experiment is provided.

Applications of DNA-stable isotope probing in bioremediation studies.

PubMed

Chen, Yin; Vohra, Jyotsna; Murrell, J Colin

2010-01-01

DNA-stable isotope probing, a method to identify active microorganisms without the prerequisite of cultivation, has been widely applied in the study of microorganisms involved in the degradation of environmental pollutants. Recent advances and technique considerations in applying DNA-SIP in bioremediation are highlighted. A detailed protocol of a DNA-SIP experiment is provided.

Beam optical design of in-flight fragment separator for high-power heavy ion beam

NASA Astrophysics Data System (ADS)

Yun, C. C.; Kim, Mi-Jung; Kim, D. G.; Song, J. S.; Kim, Myeong-Jin; Kim, J. W.; Kim, J. R.; Wan, W.

2013-12-01

An in-flight fragment separator has been designed for the rare isotope science project (RISP) in Korea. A beam used for the design is 238U in the energy of 200 MeV/u with the maximum beam power of 400 kW. The use of high-power beam requires careful removal of the primary beam by pre-separator, for which its configuration was revised to employ four dipole magnets instead of two. Different configurations of the separator have been tested in search of optimal design in non-linear optics, which was complicated by the space needed for the target, beam dump and radiation shielding. Non-linear optical calculations have been carried out using GICOSY and COSY Infinity including the fringe fields of large-aperture quadrupole magnets. Correction of non-linear terms is made with multipole coils located inside the superconducting quadrupole magnets and by external multipole magnets. Beam simulations using LISE++ and MOCADI have been performed to consider the effects of multiple charge states of the primary and isotope beams produced at the target. Layout of the separator is being finalized, and detailed optics simulation will continue to refine its design.

Laparoscopic versus open-component separation: a comparative analysis in a porcine model.

PubMed

Rosen, Michael J; Williams, Christina; Jin, Judy; McGee, Michael F; Schomisch, Steve; Marks, Jeffrey; Ponsky, Jeffrey

2007-09-01

The ideal surgical treatment for complicated ventral hernias remains elusive. Traditional component separation provides local advancement of native tissue for tension-free closure without prosthetic materials. This technique requires an extensive subcutaneous dissection with division of perforating vessels predisposing to skin-flap necrosis and complicated wound infections. A minimally invasive component separation may decrease wound complication rates; however, the adequacy of the myofascial advancement has not been studied. Five 25-kg pigs underwent bilateral laparoscopic component separation. A 10-mm incision was made lateral to the rectus abdominus muscle. The external oblique fascia was incised, and a dissecting balloon was inflated between the internal and external oblique muscles. Two additional ports were placed in the intermuscular space. The external oblique was incised from the costal margin to the inguinal ligament. The maximal abdominal wall advancement was recorded. A formal open-component separation was performed and maximal advancement 5 cm superior and 5 cm inferior to the umbilicus was recorded for comparison. Groups were compared using standard statistical analysis. The laparoscopic component separation was completed successfully in all animals, with a mean of 22 min/side. Laparoscopic component separation yielded 3.9 cm (SD 1.1) of fascial advancement above the umbilicus, whereas 4.4 cm (1.2) was obtained after open release (P = .24). Below the umbilicus, laparoscopic release achieved 5.0 cm (1.0) of advancement, whereas 5.8 cm (1.2) was gained after open release (P = .13). The minimally invasive component separation achieved an average of 86% of the myofascial advancement compared with a formal open release. The laparoscopic approach does not require extensive subcutaneous dissection and might theoretically result in a decreased incidence or decreased complexity of postoperative wound infections or skin-flap necrosis. Based on our preliminary

Lead isotope systematics of some igneous rocks from the Egyptian Shield

NASA Technical Reports Server (NTRS)

Gillespie, J. G.; Dixon, T. H.

1983-01-01

Lead isotope data on whole-rock samples and two feldspar separates for a variety of Pan-African (late Precambrian) igneous rocks for the Egyptian Shield are presented. It is pointed out that the eastern desert of Egypt is a Late Precambrian shield characterized by the widespread occurrence of granitic plutons. The lead isotope ratios may be used to delineate boundaries between Late Precambrian oceanic and continental environments in northeastern Africa. The samples belong to three groups. These groups are related to a younger plutonic sequence of granites and adamellites, a plutonic group consisting of older tonalites to granodiorites, and the Dokhan volcanic suite.

Applicability of Separation Potentials to Determining the Parameters of Cascade Efficiency in Enrichment of Ternary Mixtures

NASA Astrophysics Data System (ADS)

Palkin, V. A.; Igoshin, I. S.

2017-01-01

The separation potentials suggested by various researchers for separating multicomponent isotopic mixtures are considered. An estimation of their applicability to determining the parameters of the efficiency of enrichment of a ternary mixture in a cascade with an optimum scheme of connection of stages made up of elements with three takeoffs is carried out. The separation potential most precisely characterizing the separative power and other efficiency parameters of stages and cascade schemes has been selected based on the results of the estimation made.

Sulfur and Hydrogen Isotope Anomalies in Organic Compounds from the Murchison Meteorite

NASA Astrophysics Data System (ADS)

Cooper, G. W.; Thiemens, M. H.; Jackson, T.; Chang, S.

1995-09-01

Carbon, hydrogen and sulfur isotopic measurements have been made on individual members of a recently discovered class of organic sulfur compounds, alkyl sulfonates, in the Murchison meteorite. Cooper and Chang (1) reported the first carbon isotopic measurements of Murchison organic sulfonates, providing insight into potential synthetic mechanisms of these, and possibly other, organic species. Hydrogen isotopic measurements of the sulfonates now reveal deuterium excesses ranging from +660 to +2730 per mil. The deuterium enrichments indicate formation of the hydrocarbon portion of these compounds in a low temperature astrophysical environment consistent with that of dense molecular clouds. Measurement of the sulfur isotopes provide further constraints on the origin and mechanism of formation of these organic molecules. Recently, there has been growing documentation of sulfur isotopic anomalies in meteoritic material. Thiemens and Jackson (2) have shown that some bulk ureilites possess excess 33S and Thiemens et al. (3) have reported excess 33S in an oldhamite separate from Norton County. Rees and Thode (4) reported a large 33S excess in an Allende acid residue, however, attempts to verify this measurement have been unsuccessful, possibly due to the heterogeneous nature of the carrier phase. With the recognition that sulfur isotopes may reflect nebular chemistry, identification of potential carriers is of considerable interest. In the present study the three stable isotopes of sulfur were measured in methane sulfonate extracted from the Murchison meteorite. The isotopic composition was found to be delta 33S=2.48, delta 34S=2.49 and delta 36S = 6.76 per mil. Based upon analysis of more than 60 meteoritic, and numerous terrestrial samples, the mass fractionation lines are defined by 33Delta = delta 33S-0.50 delta 34S and 36Delta = delta 36S -1.97 delta 34S. From these relations a 33Delta = 1.24 per mil and 36Delta = 0.89 per mil is observed. These anomalies

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

Soil, the orphan hydrological compartment: evidence from O and H stable isotopes?

NASA Astrophysics Data System (ADS)

Hissler, Christophe; Legout, Arnaud; Barnich, François; Pfister, Laurent

2015-04-01

O and H stable isotopes have been successfully used for decades for studying the exchange of waters between the hydrosphere, the pedosphere and the biosphere. They greatly contribute to improve our understanding of soil-water-plant interactions. In particular, the recent hydrological concept of "two water worlds" (separation of meteoric water that infiltrates the soil as (i) mobile water, which can reach the groundwater and can enter the stream, and as (ii) tightly bound water, which is trapped in the soil microporosity and used by plants) calls for a substantial revision of our perceptual models of runoff generation. Nevertheless, there is a need for testing the applicability of this concept over a large range of ecosystemic contexts (i.e.soil and vegetation types). To date, many investigations have focused on the relationship between the various processes triggering isotope fractionation within soils. So far, the dominating perception is that the isotope profile of water observed in soils is solely due to evaporative fractionation and its shape is dependent on climate and soil parameters. However, as of today the influence of biogeochemical processes on the spatio-temporal variability of δ18O and δD of the soil solutions has been rarely quantified. O and H exchanges between soil water and other soil compartments (living organisms, minerals, exchange capacity, organic matter) remain poorly known and require deeper investigations. Eventually, we need to better understand the distribution of O and H isotopes throughout the soil matrix. In order to address these issues, we have designed and carried out two complementary isotope experiments that use one liter soil columns of a 2mm-sieved and air-dried soil. Our objectives were (1) to observe the temporal evolution of the water O and H isotopic composition starting from the field capacity to the complete drying of the soil and (2) to determine the impact of soil biogeochemical properties on the isotopic composition

MIR hollow waveguide (HWG) isotope ratio analyzer for environmental applications

NASA Astrophysics Data System (ADS)

Wang, Zhenyou; Zhuang, Yan; Deev, Andrei; Wu, Sheng

2017-05-01

An advanced commercial Mid-InfraRed Isotope Ratio (IR2) analyzer was developed in Arrow Grand Technologies based on hollow waveguide (HWG) as the sample tube. The stable carbon isotope ratio, i.e. δ13C, was obtained by measuring the selected CO2 absorption peaks in the MIR. Combined with a GC and a combustor, it has been successfully employed to measure compound specific δ13C isotope ratios in the field. By using both the 1- pass HWG and 5-path HWG, we are able to measure δ13C isotope ratio at a broad CO2 concentration of 300 ppm-37,500 ppm. Here, we demonstrate its applications in environmental studies. The δ13C isotope ratio and concentration of CO2 exhaled by soil samples was measured in real time with the isotope analyzer. The concentration was found to change with the time. We also convert the Dissolved Inorganic Carbon (DIC) into CO2, and then measure the δ13C isotope ratio with an accuracy of better than 0.3 ‰ (1 σ) with a 6 min test time and 1 ml sample usage. Tap water, NaHCO3 solvent, coca, and even beer were tested. Lastly, the 13C isotope ratio of CO2 exhaled by human beings was obtained <10 seconds after simply blowing the exhaled CO2 into a tube with an accuracy of 0.5‰ (1 σ) without sample preconditioning. In summary, a commercial HWG isotope analyzer was demonstrated to be able to perform environmental and health studies with a high accuracy ( 0.3 ‰/Hz1/2 1 σ), fast sampling rate (up to 10 Hz), low sample consumption ( 1 ml), and broad CO2 concentration range (300 ppm-37,500 ppm).

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

A Procedure to Simultaneously Determine the Calcium, Chromium, and Titanium Isotopic Compositions of Astromaterials

NASA Technical Reports Server (NTRS)

Tappa, M. J.; Simon, J. I; Jordan, M. K.; Young, E. D.

2015-01-01

Many elements display both linear (mass-dependent) and non-linear (mass-independent) isotope anomalies (relative to a common reservoir). In early Solar System objects, with the exception of oxygen, mass-dependent isotope anomalies are most commonly thought to result from phase separation processes such as evaporation and condensation, whereas many mass-independent isotope anomalies likely reflect radiogenic ingrowth or incomplete mixing of presolar components in the proto-planetary disk. Coupling the isotopic characterization of multiple elements with differing volatilities in single objects may provide information regarding the location, source material, and/or processes involved in the formation of early Solar System solids. Here, we follow up on the work presented in, and detail new procedures developed to make high-precision multi-isotope measurements of Calcium, Chromium, and Titanium with small or limited amounts of sample using thermal ionization mass spectrometry and multi-collector ICP-MS, and characterize a suite of chondritic and terrestrial standards.

Polyatomic interferences on high precision uranium isotope ratio measurements by MC-ICP-MS: Applications to environmental sampling for nuclear safeguards

DOE PAGES

Pollington, Anthony D.; Kinman, William S.; Hanson, Susan K.; ...

2015-09-04

Modern mass spectrometry and separation techniques have made measurement of major uranium isotope ratios a routine task; however accurate and precise measurement of the minor uranium isotopes remains a challenge as sample size decreases. One particular challenge is the presence of isobaric interferences and their impact on the accuracy of minor isotope 234U and 236U measurements. Furthermore, we present techniques used for routine U isotopic analysis of environmental nuclear safeguards samples and evaluate polyatomic interferences that negatively impact accuracy as well as methods to mitigate their impacts.

Recent advances in CO2 laser catalysts

NASA Technical Reports Server (NTRS)

Upchurch, B. T.; Schryer, D. R.; Brown, K. G.; Kielin, E. J.; Hoflund, G. B.; Gardner, S. D.

1991-01-01

This paper discusses several recent advances in CO2 laser catalysts including comparisons of the activity of Au/MnO2 to Pt/SnO2 catalysts with possible explanations for observed differences. The catalysts are compared for the effect of test gas composition, pretreatment temperature, isotopic integrity, long term activity, and gold loading effects on the Au/MnO2 catalyst activity. Tests conducted to date include both long-term tests of up to six months continuous operation and short-term tests of one week or more that include isotopic integrity testing.

DNA stable-isotope probing (DNA-SIP).

PubMed

Dunford, Eric A; Neufeld, Josh D

2010-08-02

DNA stable-isotope probing (DNA-SIP) is a powerful technique for identifying active microorganisms that assimilate particular carbon substrates and nutrients into cellular biomass. As such, this cultivation-independent technique has been an important methodology for assigning metabolic function to the diverse communities inhabiting a wide range of terrestrial and aquatic environments. Following the incubation of an environmental sample with stable-isotope labelled compounds, extracted nucleic acid is subjected to density gradient ultracentrifugation and subsequent gradient fractionation to separate nucleic acids of differing densities. Purification of DNA from cesium chloride retrieves labelled and unlabelled DNA for subsequent molecular characterization (e.g. fingerprinting, microarrays, clone libraries, metagenomics). This JoVE video protocol provides visual step-by-step explanations of the protocol for density gradient ultracentrifugation, gradient fractionation and recovery of labelled DNA. The protocol also includes sample SIP data and highlights important tips and cautions that must be considered to ensure a successful DNA-SIP analysis.

Age determination of single plutonium particles after chemical separation

NASA Astrophysics Data System (ADS)

Shinonaga, T.; Donohue, D.; Ciurapinski, A.; Klose, D.

2009-01-01

Age determination of single plutonium particles was demonstrated using five particles of the standard reference material, NBS 947 (Plutonium Isotopic Standard. National Bureau of Standards, Washington, D.C. 20234, August 19, 1982, currently distributed as NBL CRM-137) and the radioactive decay of 241Pu into 241Am. The elemental ratio of Am/Pu in Pu particles found on a carbon planchet was measured by wavelength dispersive X-ray spectrometry (WDX) coupled to a scanning electron microscope (SEM). After the WDX measurement, each plutonium particle, with an average size of a few μm, was picked up and relocated to a silicon wafer inside the SEM chamber using a micromanipulator. The silicon wafer was then transferred to a quartz tube for dissolution in an acid solution prior to chemical separation. After the Pu was chemically separated from Am and U, the isotopic ratios of Pu ( 240Pu/ 239Pu, 241Pu/ 239Pu and 242Pu/ 239Pu) were measured with a thermal ionization mass spectrometer (TIMS) for the calculation of Pu age. The age of particles determined in this study was in good agreement with the expected age (35.9 a) of NBS 947 within the measurement uncertainty.

Uncoupling between soil and xylem water isotopic composition: how to discriminate mobile and tightly-bound water?

NASA Astrophysics Data System (ADS)

Martín Gómez, Paula; Aguilera, Mònica; Pemán, Jesús; Gil Pelegrín, Eustaquio; Ferrio, Juan Pedro

2014-05-01

As a general rule, no isotopic fractionation occurs during water uptake and water transport, thus, xylem water reflects source water. However, this correspondence does not always happen. Isotopic enrichment of xylem water has been found in several cases and has been either associated to 'stem processes' like cuticular evaporation 1 and xylem-phloem communication under water stress 2,3 or to 'soil processes' such as species-specific use of contrasting water sources retained at different water potential forces in soil. In this regard, it has been demonstrated that mobile and tightly-bound water may show different isotopic signature 4,5. However, standard cryogenic distillation does not allow to separate different water pools within soil samples. Here, we carried out a study in a mixed adult forest (Pinus sylvestris, Quercus subpyrenaica and Buxus sempervirens) growing in a relatively deep loamy soil in the Pre-Pyrenees. During one year, we sampled xylem from twigs and soil at different depths (10, 30 and 50 cm). We also sampled xylem from trunk and bigger branches to assess whether xylem water was enriched in the distal parts of the tree. We found average deviations in the isotopic signature from xylem to soil of 4o 2o and 2.4o in δ18O and 18.3o 7.3o and 8.9o in δ2H, for P.sylvestris, Q.subpyrenaica and B.sempervirens respectively. Xylem water was always enriched compared to soil. In contrast, we did not find clear differences in isotopic composition between xylem samples along the tree. Declining the hypothesis that 'stem processes' would cause these uncoupling between soil and xylem isotopic values, we tested the possibility to separate mobile and tightly-bound water by centrifugation. Even though we could separate two water fractions in soils close to saturation, we could not recover a mobile fraction in drier soils. In this regard, we welcome suggestions on alternatives to separate different soil fractions in order to find the correspondence between soil and

Signal or noise? Separating grain size-dependent Nd isotope variability from provenance shifts in Indus delta sediments, Pakistan

NASA Astrophysics Data System (ADS)

Jonell, T. N.; Li, Y.; Blusztajn, J.; Giosan, L.; Clift, P. D.

2017-12-01

Rare earth element (REE) radioisotope systems, such as neodymium (Nd), have been traditionally used as powerful tracers of source provenance, chemical weathering intensity, and sedimentary processes over geologic timescales. More recently, the effects of physical fractionation (hydraulic sorting) of sediments during transport have called into question the utility of Nd isotopes as a provenance tool. Is source terrane Nd provenance resolvable if sediment transport strongly induces noise? Can grain-size sorting effects be quantified? This study works to address such questions by utilizing grain size analysis, trace element geochemistry, and Nd isotope geochemistry of bulk and grain-size fractions (<63μm, 63-125 μm, 125-250 μm) from the Indus delta of Pakistan. Here we evaluate how grain size effects drive Nd isotope variability and further resolve the total uncertainties associated with Nd isotope compositions of bulk sediments. Results from the Indus delta indicate bulk sediment ɛNd compositions are most similar to the <63 µm fraction as a result of strong mineralogical control on bulk compositions by silt- to clay-sized monazite and/or allanite. Replicate analyses determine that the best reproducibility (± 0.15 ɛNd points) is observed in the 125-250 µm fraction. The bulk and finest fractions display the worst reproducibility (±0.3 ɛNd points). Standard deviations (2σ) indicate that bulk sediment uncertainties are no more than ±1.0 ɛNd points. This argues that excursions of ≥1.0 ɛNd points in any bulk Indus delta sediments must in part reflect an external shift in provenance irrespective of sample composition, grain size, and grain size distribution. Sample standard deviations (2s) estimate that any terrigenous bulk sediment composition should vary no greater than ±1.1 ɛNd points if provenance remains constant. Findings from this study indicate that although there are grain-size dependent Nd isotope effects, they are minimal in the Indus delta such

Tracing the pathways of neotropical migratory shorebirds using stable isotopes: a pilot study.

PubMed

Farmer, A; Rye, R; Landis, G; Bern, C; Kester, C; Ridley, I

2003-09-01

We evaluated the potential use of stable isotopes to establish linkages between the wintering grounds and the breeding grounds of the Pectoral Sandpiper (Calidris melanotos), the White-rumped Sandpiper (Calidris fuscicollis), the Baird's Sandpiper (Calidris bairdii), and other Neotropical migratory shorebird species (e.g., Tringa spp.). These species molt their flight feathers on the wintering grounds and hence their flight feathers carry chemical signatures that are characteristic of their winter habitat. The objective of our pilot study was to assess the feasibility of identifying the winter origin of individual birds by: (1) collecting shorebird flight feathers from several widely separated Argentine sites and analyzing these for a suite of stable isotopes; and 2) analyzing the deuterium and 18O isotope data that were available from precipitation measurement stations in Argentina. Isotopic ratios (delta13C, delta15N and delta34S) of flight feathers were significantly different among three widely separated sites in Argentina during January 2001. In terms of relative importance in separating the sites, delta34S was most important, followed by delta15N, and then delta13C. In the complete discriminant analysis, the classification function correctly predicted group membership in 85% of the cases (jackknifed classification matrix). In a stepwise analysis delta13C was dropped from the solution, and site membership was correctly predicted in 92% of cases (jackknifed matrix). Analysis of precipitation data showed that both deltaD and delta18O were significantly related to both latitude and longitude on a countrywide scale (p < 0.001). Other variables, month, altitude, explained little additional variation in these isotope ratios. Several issues were identified that will likely constrain the degree of accuracy one can expect in predicting the geographic origin of birds from Argentina. There was unexplained variation in isotope ratios within and among the different wing

Tracing the pathways of Neotropical migratory shorebirds using stable isotopes: A pilot study

USGS Publications Warehouse

Farmer, A.H.; Rye, R.; Landis, G.; Bern, C.; Kester, C.; Ridley, I.

2003-01-01

We evaluated the potential use of stable isotopes to establish linkages between the wintering grounds and the breeding grounds of the Pectoral Sandpiper (Calidris melanotos), the White-rumped Sandpiper (Calidris fuscicollis), the Baird's Sandpiper (Calidris bairdii), and other Neotropical migratory shorebird species (e.g., Tringa spp.). These species molt their flight feathers on the wintering grounds and hence their flight feathers carry chemical signatures that are characteristic of their winter habitat. The objective of our pilot study was to assess the feasibility of identifying the winter origin of individual birds by: (1) collecting shorebird flight feathers from several widely separated Argentine sites and analyzing these for a suite of stable isotopes; and (2) analyzing the deuterium and 18O isotope data that were available from precipitation measurement stations in Argentina. Isotopic ratios (δ13C, δ15N and δ34S) of flight feathers were significantly different among three widely separated sites in Argentina during January 2001. In terms of relative importance in separating the sites, δ34S was most important, followed by δ15N, and then δ13C. In the complete discriminant analysis, the classification function correctly predicted group membership in 85% of the cases (jackknifed classification matrix). In a stepwise analysis δ13C was dropped from the solution, and site membership was correctly predicted in 92% of cases (jackknifed matrix). Analysis of precipitation data showed that both δD and δ18O were significantly related to both latitude and longitude on a countrywide scale (p < 0.001). Other variables, month, altitude, explained little additional variation in these isotope ratios. Several issues were identified that will likely constrain the degree of accuracy one can expect in predicting the geographic origin of birds from Argentina. There was unexplained variation in isotope ratios within and among the different wing feathers from individual

Mo isotope fractionation during hydrothermal evolution of porphyry Cu systems

NASA Astrophysics Data System (ADS)

Shafiei, Behnam; Shamanian, GholamHossein; Mathur, Ryan; Mirnejad, Hassan

2015-03-01

We present Mo isotope compositions of molybdenite types from three successive stages of ore deposition in several porphyry copper deposits of the Kerman region, Iran. The data provide new insights into controlling processes on Mo isotope fractionation during the hydrothermal evolution of porphyry systems. The Mo isotope compositions of 27 molybdenite samples show wide variations in δ97Mo ranging from -0.37 to +0.92 ‰. The data reveal that molybdenites in the early and transitional stages of mineralization (preferentially 2H polytypes; δ97Mo mean = 0.35 ‰) have higher δ97Mo values than late stage (mainly 3R polytypes; δ97Mo mean = 0.02 ‰) molybdenites. This trend suggests that fractionation of Mo isotopes occurred in high-temperature stages of mineralization and that hydrothermal systems generally evolve towards precipitation of molybdenite with lower δ97Mo values. Taking into account the genetic models proposed for porphyry Cu deposits along with the temperature-dependent fractionation of Mo isotope ratios, it is proposed that large variations of Mo isotopes in the early and the transitional stages of ore deposition could be controlled by the separation of the immiscible ore-forming fluid phases with different density, pH, and ƒO2 properties (i.e., brine and vapor). The fractionation of Mo isotopes during fluid boiling and Rayleigh distillation processes likely dominates the Mo isotope budget of the remaining ore-forming fluids for the late stage of mineralization. The lower δ97Mo values in the late stage of mineralization can be explained by depletion of the late ore-forming hydrothermal solutions in 97Mo, as these fluids have moved to considerable distance from the source. Finally, the relationship observed between MoS2 polytypes (2H and 3R) and their Mo isotopic compositions can be explained by the molecular vibration theory, in which heavier isotopes are preferentially partitioned into denser primary 2H MoS2 crystals.

Can Biomass Burning Explain Isotopically Light Fe in Marine Aerosols?

NASA Astrophysics Data System (ADS)

Sherry, A. M.; Anbar, A. D.; Herckes, P.; Romaniello, S. J.

2016-02-01

Iron (Fe) is an important micronutrient that limits primary productivity in large parts of the ocean. In these regions, atmospheric aerosol deposition is an important source of Fe to the surface ocean and thus has a critical impact on ocean biogeochemistry. Fe-bearing aerosols originate from many sources with potentially distinct Fe isotopic compositions. Consequently, Fe isotopes may provide a new tool to trace the sources of aerosol Fe to the oceans. Mead et al. (2013) first discovered that Fe in the fine fraction of Bermuda aerosols is often isotopically lighter than Fe from known anthropogenic and crustal sources. 1 These authors suggested that this light isotopic signature was likely the result of biomass burning, since Fe in plants is the only known source of isotopically light Fe. More recently, Conway et al. found that Fe in the soluble fraction of aerosols collected during 2010-2011 North Atlantic GEOTRACES cruises also showed light isotope values, which they likewise attributed to biomass burning.2 These studies are further supported by new modeling work which suggests that biomass burning aerosols should contribute significant amounts of soluble Fe to tropical and southern oceans.3To test if biomass burning releases aerosols with a light Fe isotope composition, we are conducting lab-scale biomass burning experiments using natural samples of vegetation and leaf litter. Burn aerosols were collected on cellulose filters, then digested and analyzed for trace metal concentrations using inductively-coupled mass spectrometry (ICP-MS). Fe isotopes were determined by using multiple collector ICP-MS following separation and purification of Fe using anion exchange chromatography. We will discuss metal concentration and isotope data from these experiments with implications for the interpretation of Fe isotope signals in aerosol samples. 1Mead, C et al. GRL, 2013, 40, 5722-5727. 2 Conway, T et al. Goldschmidt Abs 2015 593. 3Ito, A. ES&T Lett, 2015, 2, 70-75.

A comparison of lead-isotope measurements on exploration-type samples using inductively coupled plasma and thermal ionization mass spectrometry

USGS Publications Warehouse

Gulson, B.L.; Meier, A.L.; Church, S.E.; Mizon, K.J.

1989-01-01

Thermal ionization mass spectrometry (TI-MS) has long been the method of choice for Pb-isotope determinations. More recently, however, inductively coupled plasma mass spectrometry (ICP-MS) has been used to determine Pb-isotope ratios for mineral exploration. The ICP-MS technique, although not as precise as TI-MS, may promote a wider application of Ph-isotope ratio methods because it allows individual isotopes to be determined more rapidly, generally without need for chemical separation (e.g., Smith et al., 1984; Hinners et al., 1987). To demonstrate the utility of the ICP-MS method, we have conducted a series of Pb-isotope measurements on several suites of samples using both TI-MS and ICP-MS. ?? 1989.

The Nuclear Energy Advanced Modeling and Simulation Safeguards and Separations Reprocessing Plant Toolkit

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCaskey, Alex; Billings, Jay Jay; de Almeida, Valmor F

2011-08-01

This report details the progress made in the development of the Reprocessing Plant Toolkit (RPTk) for the DOE Nuclear Energy Advanced Modeling and Simulation (NEAMS) program. RPTk is an ongoing development effort intended to provide users with an extensible, integrated, and scalable software framework for the modeling and simulation of spent nuclear fuel reprocessing plants by enabling the insertion and coupling of user-developed physicochemical modules of variable fidelity. The NEAMS Safeguards and Separations IPSC (SafeSeps) and the Enabling Computational Technologies (ECT) supporting program element have partnered to release an initial version of the RPTk with a focus on software usabilitymore » and utility. RPTk implements a data flow architecture that is the source of the system's extensibility and scalability. Data flows through physicochemical modules sequentially, with each module importing data, evolving it, and exporting the updated data to the next downstream module. This is accomplished through various architectural abstractions designed to give RPTk true plug-and-play capabilities. A simple application of this architecture, as well as RPTk data flow and evolution, is demonstrated in Section 6 with an application consisting of two coupled physicochemical modules. The remaining sections describe this ongoing work in full, from system vision and design inception to full implementation. Section 3 describes the relevant software development processes used by the RPTk development team. These processes allow the team to manage system complexity and ensure stakeholder satisfaction. This section also details the work done on the RPTk ``black box'' and ``white box'' models, with a special focus on the separation of concerns between the RPTk user interface and application runtime. Section 4 and 5 discuss that application runtime component in more detail, and describe the dependencies, behavior, and rigorous testing of its constituent components.« less

Advanced oxidative processes and membrane separation for micropollutant removal from biotreated domestic wastewater.

PubMed

Silva, Larissa L S; Sales, Julio C S; Campos, Juacyara C; Bila, Daniele M; Fonseca, Fabiana V

2017-03-01

The presence of micropollutants in sewage is already widely known, as well as the effects caused by natural and synthetic hormones. Thus, it is necessary to apply treatments to remove them from water systems, such as advanced oxidation processes (AOPs) and membrane separation processes, which can oxidize and remove high concentrations of organic compounds. This work investigated the removal of 17β-estradiol (E2), 17α-ethinylestradiol (EE2), and estriol (E3) from biotreated sewage. Reverse osmosis processes were conducted at three recoveries (50, 60, and 70 %). For E2 and EE2, the removals were affected by the recovery. The best results for RO were as follows: the E2 compound removal was 89 % for 60 % recovery and the EE2 compound removal was 57 % for 50 % recovery. The RO recovery did not impact the E3 removal. It was concluded that the interaction between the evaluated estrogens, and the membrane was the major factor for the hormone separation. The AOP treatment using H 2 O 2 /UV was carried out in two sampling campaigns. First, we evaluated the variation of UV doses (24.48, 73.44, 122.4, and 244.8 kJ m -2 ) with 18.8 mg L -1 of H 2 O 2 in the reaction. EE2 showed considerable removals (around 70 %). In order to optimize the results, an experimental design was applied. The best result was obtained with higher UV dose (122.4 kJ m -2 ) and lower H 2 O 2 concentration (4 mg L -1 ), achieving removal of 91 % for E3 and 100 % for E2 and EE2.

Stable isotope paleoaltimetry and the evolution of landscapes and life

NASA Astrophysics Data System (ADS)

Mulch, Andreas

2016-01-01

Reconstructing topography of our planet not only advances our knowledge of the geodynamic processes that shape the Earth's surface; equally important it adds a key element towards understanding long-term continental moisture transport, atmospheric circulation and the distribution of biomes and biodiversity. Stable isotope paleoaltimetry exploits systematic decreases in the oxygen (δ18O) or hydrogen (δD) isotopic composition of precipitation along a mountain front when the interaction of topography and advected moist air masses induces orographic precipitation. These changes in δ18O or δD can be recovered from the geologic record and recent geochemical and modeling advances allow a broad range of proxy materials to be evaluated. Over the last 10 yr stable isotope paleoaltimetry has witnessed rapidly expanding research activities and has produced a broad array of fascinating tectonic and geomorphologic studies many of which have concentrated on determining the elevation history of continental plateau regions. These single-site studies have greatly expanded what used to be very sparse global paleoaltimetric data. The challenge now lies in disentangling the surface uplift component from the impact of climate change on δ18O and δD in precipitation. The robustness of stable isotope paleoaltimetry can be enhanced when high-elevation δ18O or δD data are referenced against low-elevation sites that track climate-modulated sea level δ18O or δD of precipitation through time (' δ- δ approach'). Analysis of central Andean paleosols documents that differences in δ18O of soil carbonate between the Subandean foreland and the Bolivian Altiplano are small between 11 and 7 Ma but rise rapidly to ca. 2.9‰ after 7 Ma, corroborating the magnitude of late Miocene change in δ18O on the Altiplano. Future advances in stable isotope paleoaltimetry will greatly benefit from addressing four key challenges: (1) Identifying topographically-induced changes in atmospheric

Compound Specific Hydrogen Isotope Composition of Type II and III Kerogen Extracted by Pyrolysis-GC-MS-IRMS

NASA Technical Reports Server (NTRS)

Socki, Richard A.; Pernia, Denet; Evans, Michael; Fu, Qi; Bissada, Kadry K.; Curiale, Joseph A.; Niles, Paul B.

2013-01-01

The use of Hydrogen (H) isotopes in understanding oil and gas resource plays is in its infancy. Described here is a technique for H isotope analysis of organic compounds pyrolyzed from oil and gas shale-derived kerogen. Application of this technique will progress our understanding. This work complements that of Pernia et al. (2013, this meeting) by providing a novel method for the H isotope analysis of specific compounds in the characterization of kerogen extracted by analytically diverse techniques. Hydrogen isotope analyses were carried out entirely "on-line" utilizing a CDS 5000 Pyroprobe connected to a Thermo Trace GC Ultra interfaced with a Thermo MAT 253 IRMS. Also, a split of GC-separated products was sent to a DSQ II quadrupole MS to make semi-quantitative compositional measurements of the extracted compounds. Kerogen samples from five different basins (type II and III) were dehydrated (heated to 80 C overnight in vacuum) and analyzed for their H isotope compositions by Pyrolysis-GC-MS-TC-IRMS. This technique takes pyrolysis products separated via GC and reacts them in a high temperature conversion furnace (1450 C) which quantitatively forms H2, following a modified method of Burgoyne and Hayes, (1998, Anal. Chem., 70, 5136-5141). Samples ranging from approximately 0.5 to 1.0mg in size, were pyrolyzed at 800 C for 30s. Compounds were separated on a Poraplot Q GC column. Hydrogen isotope data from all kerogen samples typically show enrichment in D from low to high molecular weight compounds. Water (H2O) average deltaD = -215.2 (V-SMOW), ranging from -271.8 for the Marcellus Shale to -51.9 for the Polish Shale. Higher molecular weight compounds like toluene (C7H8) have an average deltaD of -89.7 0/00, ranging from -156.0 for the Barnett Shale to -50.0 for the Monterey Shale. We interpret these data as representative of potential H isotope exchange between hydrocarbons and sediment pore water during formation within each basin. Since hydrocarbon H isotopes