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FY-12 INL KR CAPTURE ACTIVITIES SUPPORTING THE OFF-GAS SIGMA TEAM

Description: Tasks performed this year by INL Kr capture off-gas team members can be segregated into three separate task sub-sections which include: 1) The development and testing of a new engineered form sorbent, 2) An initial NDA gamma scan effort performed on the drum containing the Legacy Kr-85 sample materials, and 3) Collaborative research efforts with PNNL involving the testing of the Ni-DOBDC MOF and an initial attempt to make powdered chalcogel material into an engineered form using our binding process. This document describes the routes to success for the three task sub-sections.
Date: August 1, 2012
Creator: Garn, Troy G.; Greenhalgh, Mitchell R. & Law, Jack D
Partner: UNT Libraries Government Documents Department

Novel Sorbent Development and Evaluation for the Capture of Krypton and Xenon from Nuclear Fuel Reprocessing Off-Gas Streams

Description: The release of volatile radionuclides generated during Used Nuclear Fuel reprocessing in the US will most certainly need to be controlled to meet US regulatory emission limits. A US DOE sponsored Off-Gas Sigma Team has been tasked with a multi-lab collaborative research and development effort to investigate and evaluate emissions and immobilization control technologies for the volatile radioactive species generated from commercial Used Nuclear Fuel (UNF) Reprocessing. Physical Adsorption technology is a simpler and potential economical alternative to cryogenic distillation processes that can be used for the capture of krypton and xenon and has resulted in a novel composite sorbent development procedure using synthesized mordenite as the active material. Utilizing the sorbent development procedure, INL sigma team members have developed two composite sorbents that have been evaluated for krypton and xenon capacities at ambient and 191 K temperature using numerous test gas compositions. Adsorption isotherms have been generated to predict equilibration and maximum capacities enabling modeling to support process equipment scale-up.
Date: October 1, 2013
Creator: Garn, Troy G.; Greenhalgh, Mitchell R. & Law, Jack D.
Partner: UNT Libraries Government Documents Department

Novel Sorbent Development and Evaluation for the Capture of Krypton and Xenon from Nuclear Fuel Reprocessing Off-Gas Streams

Description: The release of volatile radionuclides generated during Used Nuclear Fuel reprocessing in the US will most certainly need to be controlled to meet US regulatory emission limits. A US DOE sponsored Off-Gas Sigma Team has been tasked with a multi-lab collaborative research and development effort to investigate and evaluate emissions and immobilization control technologies for the volatile radioactive species generated from commercial Used Nuclear Fuel (UNF) Reprocessing. Physical Adsorption technology is a simpler and potential economical alternative to cryogenic distillation processes that can be used for the capture of krypton and xenon and has resulted in a novel composite sorbent development procedure using synthesized mordenite as the active material. Utilizing the sorbent development procedure, INL sigma team members have developed two composite sorbents that have been evaluated for krypton and xenon capacities at ambient and 191 K temperature using numerous test gas compositions. Adsorption isotherms have been generated to predict equilibration and maximum capacities enabling modeling to support process equipment scale-up.
Date: September 1, 2013
Creator: Garn, Troy G.; Greenhalgh, Mitchell R. & Law, Jack D.
Partner: UNT Libraries Government Documents Department

Photon burst mass spectrometry--ultrasensitive detection of rare isotopes

Description: Progress is reported on the development of a new technique for measurement of trace levels of radioisotopes which is based on fluorescence detection of output from a mass spectrometer. Significant achievements include the observation of fluorescence and burst signals from Kr isotopes, including enriched samples of {sup 85}Kr with a 4-collector system. An abundance sensitivity is demonstrated with {sup 83}Kr and {sup 85}Kr.
Date: February 1, 1995
Creator: Hansen, C.S.; Pan, X.J.; Fairbank, W.M. Jr.; Oona, H.; Chamberlin, E.P.; Nogar, N.S. et al.
Partner: UNT Libraries Government Documents Department

FT-ICR mass spectrometry of very highly charged atomic ions

Description: The authors report FT-ICR measurements of samples trapped in the electron beam ion trap (EBIT) at Livermore. They made use of the access provided by the radial x-ray slots. They constructed two probes that could be inserted into the 2-mm wide slots. The probes each subtend only 25{degree} and face each other 180{degree} apart. They show a typical transformed spectrum of highly charged {sup 84}Kr ions obtained with this system. The spectrum was obtained by exciting with a 300-{mu}s sweep from 17.5 to 19.5 MHz. The resonance peaks of {sup 84}Kr{sup 34+}, {sup 84}Kr{sup 35+}, and {sup 84}Kr{sup 36+} are clearly visible.
Date: May 15, 1995
Creator: Schweikhard, L.; Beck, B. & Beiersdorfer, P.
Partner: UNT Libraries Government Documents Department

Model Calculations of Continuous-Wave Laser Ionization of Krypton

Description: This report describes modeling of a scheme that uses continuous-wave (CW) lasers to ionize selected isotopes of krypton with high isotopic selectivity. The models predict that combining this ionization scheme with mass spectrometric measurement of the resulting ions can be the basis for ultra-sensitive methods to measure {sup 85}Kr in the presence of a 10{sup 11} excess of the stable krypton isotopes. Two experimental setups are considered in this model: the first setup is for krypton as a static gas, the second is for krypton in an atomic beam. In the static gas experiment, for a total krypton press of 10{sup {minus}4} torr and 10 W of power in the cavity, the model predicts a total krypton ion current of 4.6 x 10{sup 8} s{sup {minus}1} and for a {sup 85}Kr/Kr of 10{sup {minus}11} a {sup 85}Kr ion current of 3.5 s{sup {minus}1} or about 10,000 per hour. The atomic beam setup allowed higher isotopic selectivity; the model predicts a {sup 85}Kr ion current of 18 s{sup {minus}1} or 65,000 per hour.
Date: July 27, 1999
Creator: Cannon, Bret D.
Partner: UNT Libraries Government Documents Department

Alternative Bench Standards: Sample Production Report

Description: The INL has prepared four standards representing krypton concentrations of 1.1X, 1.54X, 10X and 100X the reported atmospheric value of 70 dpm 85Kr per cubic centimeter of Kr gas at 25 degrees C (ie. 1.1X is 1.1 x 70, or 77 dpm 85Kr per cubic centimeter of Kr gas at 25 degrees C). A t-zero date and time of January 1, 2012 at 1200 Zulu was used for all standards. The Alternative Bench Standards (ABS) of 1.1X, 1.54X, 10X and 100X, are designated by titles of ABS-A, ABS-B, ABS C and ABS-D, respectively. The concentration of Kr in air is 1.14 ppm.
Date: September 1, 2012
Creator: Mann, N. R.; Houghton, T. P.; Watrous, M. G.; Eisenmenger, J. G. & Hague, R. K.
Partner: UNT Libraries Government Documents Department

Up-Dating Of Atomic Data Needed For Ionisation Balance Evaluations of Krypton and Molybdenum

Description: Atomic data for both ionization and recombination of Kr and Mo ions are reviewed, since the rate coefficients for these processes need to be regularly up-dated following the publication of new theoretical calculations and new experimental data. Kr is used in magnetic-confinement-fusion devices to produce a peripheral radiating mantle meant to spread the heat confinement-load on the plasma-facing components. In a few tokamaks Mo tiles cover the plasma-facing surfaces, acting in most cases as a plasma-column limiter. The collected atomic data represent the state of the art on the ionization and recombination data for the two considered elements. Samples of rates are proposed for both ionization and recombination along with tables of the fractional abundances at ionization equilibrium. The proposed rates should be included in codes that simulate the impurity behavior in magnetic-confinement-fusion devices, i.e., when radial transport is added to ionization and recombination to predict spatially resolved charge-state distributions that are to be compared with experimental results.
Date: June 1, 2006
Creator: Mattioli, M; Mazzitelli, G; Fournier, K B; Finkenthal, M & Carraro, L
Partner: UNT Libraries Government Documents Department

[Photon burst mass spectrometry technique.] Final report

Description: The basic tools have been developed and demonstrated for selective detection of Kr isotopes in the Photon Burst Mass Spectrometry technique. The effort is divided into: photon burst measurements on Mg{sup +} demonstrating high isotopic selectivity, charge exchange of Kr{sup +} with Cs and Rb to produce metastable Kr atoms, development of a diode laser system for photon burst detection of Kr{sup +}, and measurements of photon bursts detection of Kr.
Date: April 1, 1996
Creator: Fairbank, W.M. Jr
Partner: UNT Libraries Government Documents Department

Photoelectron angular distributions beyond the dipole approximation

Description: This paper reports the measurement of nondipolar asymmetry parameters for the angular distributions of Ar 1s, Kr 2s, and Kr 2p photoemission within 2-3 keV above their respective thresholds. Pronounced asymmetries with respect to direction of photon propagation are present even at low electron kinetic energies. The energy dependence of the asymmetry is Z- and subshell-specific and causes the direction of preferred electron emission to change sign at least once in each case. Towards higher energies, the asymmetry increases and the photoelectron emission pattern is forward-skewed for all 3 cases. Measured asymmetry parameters are in good agreement with recent predictions from nonrelativistic calculations which include interference between electric-dipole and electric-quadrupole transition amplitudes in the photoabsorption process.
Date: August 1996
Creator: Kraessig, B.; Jung, M.; Gemmell, D. S.; Kanter, E. P.; LeBrun, T.; Southworth, S. H. et al.
Partner: UNT Libraries Government Documents Department

Development of laser-based resonance ionization techniques for 81-Kr and 85-Kr measurements in the geosciences, II. December 1, 1994 through December 31, 2000 reporting period. Final technical report for Grant No. DE-FG05-95ER14497

Description: A facility for measurement of rare Kr-81 and Kr-85 isotope concentration in hydrogeologic samples, and isotopic composition of minute quantities of krypton and xenon from extraterrestrial samples, was established, requiring refinement of an emerging mass spectrometric-based analytical technique and securing of laboratory space and equipment. The analytical process consists of (1) collecting a groundwater sample, (2) degassing the water, (3) separating Kr from the recovered gases, (4&5) two isotopic enrichments to reduce interfering isotopes by E9, and (6) detecting the rare krypton isotope in a unique time-of-flight mass spectrometer detecting as few as 100 Kr atoms. All equipment is installed and operating, with only some additional adjustment and testing of the last step (6, above) remaining to be completed. Collaborations have been established with a number of researchers and organizations world wide, and both groundwater and extraterrestrial samples have been collected. Completion of analyses awaits full operation of step 6.
Date: February 5, 2001
Creator: Thonnard, Norbert; McKay, Larry D. & Labotka, Theodore C.
Partner: UNT Libraries Government Documents Department

Production of Xe¹³¹, Xe¹³⁵, Kr⁸⁵m and Kr⁸⁵ From Plated-Out U²³⁵ in the MTR Core

Description: This report discusses details of the release of Xe¹³¹, Xe¹³⁵, Kr⁸⁵m and Kr⁸⁵ into the process water system of the MTR along with the development of high process water radioactivity. It is suggested that this release followed the fissioning of U²³⁵. Equations that produce the rate of release of fission products is given and approximate rate of release is represented in a graph.
Date: January 14, 1955
Creator: Grimaud, Adrian V.
Partner: UNT Libraries Government Documents Department

Atom trap trace analysis of krypton isotopes

Description: A new method of ultrasensitive isotope trace analysis has been developed. This method, based on the technique of laser manipulation of neutral atoms, has been used to count individual {sup 85}Kr and {sup 81}Kr atoms present in a natural krypton gas sample with isotopic abundances in the range of 10{sup {minus}11} and 10{sup {minus}13}, respectively. This method is free of contamination from other isotopes and elements and can be applied to several different isotope tracers for a wide range of applications. The demonstrated detection efficiency is 1 x 10{sup {minus}7}. System improvements could increase the efficiency by many orders of magnitude.
Date: November 17, 1999
Creator: Bailey, K.; Chen, C. Y.; Du, X.; Li, Y. M.; Lu, Z.-T.; O'Connor, T. P. et al.
Partner: UNT Libraries Government Documents Department

Atom trap trace analysis

Description: A new method of ultrasensitive trace-isotope analysis has been developed based upon the technique of laser manipulation of neutral atoms. It has been used to count individual {sup 85}Kr and {sup 81}Kr atoms present in a natural krypton sample with isotopic abundances in the range of 10{sup {minus}11} and 10{sup {minus}13}, respectively. The atom counts are free of contamination from other isotopes, elements,or molecules. The method is applicable to other trace-isotopes that can be efficiently captured with a magneto-optical trap, and has a broad range of potential applications.
Date: May 25, 2000
Creator: Lu, Z.-T.; Bailey, K.; Chen, C.-Y.; Du, X.; Li, Y.-M.; O'Connor, T. P. et al.
Partner: UNT Libraries Government Documents Department

Noble gas isotope measurements for spent nuclear fuel reprocessing. IAEA Task 90/0A211 interim report

Description: The nuclear fission of actinides in reactor fuel produces large quantities of Kr and Xe as fission products. Because of the high levels of fission Kr and Xe, sample collection and analysis of noble gases for spent fuel diagnostic measurements is a simple, straight-forward technique. In modern reprocessing plants with continuous dissolvers, it will not be possible to use traditional methods for isolating input batches of fuel. This study investigates the feasibility of using noble gas isotope abundance measurements (isotope correlation techniques - ICT) to solve safeguards requirements. Noble gas measurements might be able to provide an independent analysis of Pu contained within dissolves fuel, on an individual fuel assembly basis. The isotopic composition of Kr and Xe in spent fuel reflects both the composition (isotope abundance ratios) of the fission products and the effects of neutron capture on those fission products. We have reviewed the available literature for noble gas analyses of spent reactor fuel. While references are made to noble gas isotope correlations over the last 20 years, we have found little if any detailed analysis of large data sets. The literature search did find several useful reports. Of these papers, one is particularly useful for evaluating noble gas isotopic compositions. The ``Benchmark-paper`` (1) contains 54 Kr and 56 Xe isotopic composition analyses for 4 different reactors with a variety of fuel enrichment factors. Burnup ranges from 8000 to 37000 MWd/tU. Besides the noble gas measurements, a variety of other measurements are reported (actinides and fission products).
Date: February 17, 1993
Creator: Hudson, G. B.
Partner: UNT Libraries Government Documents Department