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Actinide determination and analytical support for characterization of environmental samples

TL;DR: Clean chemical and thermal ionization mass spectrometry (TIMS) procedures have been developed to permit the determination of environmental actinide element concentrations and isotopic signatures as discussed by the authors.
Abstract: Clean chemical and Thermal Ionization Mass Spectrometry (TIMS) procedures have been developed to permit the determination of environmental actinide element concentrations and isotopic signatures. The isotopic signatures help identify element origin and separate naturally occurring or background contributions from local anthropogenic sources. Typical sample sizes for processing are 2 liters of water, 1--10 grams of sediment, and 1--20 grams of soil. Measurement limits for Pu, Am, and Np are < 1 {times} 18{sup 8} atoms, and for U are < 2.5 {times} 10{sup 12} atoms. For isotopic signatures, < 5 {times} 10{sup 8} atoms of Pu, Am, and Np are necessary, and 8 {times} 10{sup 12} atoms of U are required. Of potential interest to the IAEA is the incorporation of these techniques into their Safeguards Analytical Laboratory for environmental sampling. Studies made of surface waters, sediments and soils from the Rocky Flats Plant (RFP) in Colorado, US, are used as examples of this methodology. These studies showed that, although plant boundary actinide concentrations approached, on the downstream side, natural or background levels, isotopic signatures characteristic of plant operations were still discernible.

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LA-UR-94- 9 _ " 0 4; 6 g
Titlo: "ACTINIDE DETERMINATION AND ANALYTICAL
• SUPPORT FOR CHARACTERIZATION OF
ENVIRONMENTAL SAMPLES"
Author(s): Donald J. Rokop, Deward W. Efurd, Richard E. Perrin
Los Alamos
NATIONAL LABORATORY
Los Alamos National Laboratory, an affirmative action/equal opportunity employer, is operated by the University of California for the U.S. Department of Energy
under contract W-7405-ENG-36, By acceptance of _is article, the publisher recognize_ that the U.S. Governmm!.! r_t,pinjLa_,'_nlp_clyNue, ,,fG_lf,alty-free license to
publish or reproduce the published form of this contribution, or to allow others to do so, for U.S. Government puf_,_s, _hp _.e_14J_ho__'N_ti_ Laboralory
requests that the publisher identify this article as work performed under the auspices of the. U.S. Department of _r_etgy. '. '- " _ 4"
FormNo.836 R5
HAR0 8 1994

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ACTINIDE DETERMINATIONAND ANALYTICAL SUPPORT FOR
CHARACTERIZATIONOF ENVIRONMENTALSAMPLES
Donald J. Rokop,DewardW. Efurd,anti,RichardE. Perrin*
ChemicalScienceand TechnologyDivision
LosAlamosNationalLaboratory
LosAlamos,New Mexico USA
* NowwithRadianCorporation
' White Rock,New Mexico USA

' IAEA-SM-333/99
ACTINIDE DETERMINATIONAND ANALYTICAL SUPPORT FOR
CHARACTERIZATION OF ENVIRONMENTALSAMPLES
ABSTRACT
Clean chemical and Thermal Ionization Mass Spectrometry (TIMS) procedures have
been developed to permit the determination of environmental actinide element
concentrations and isotopic signatures. The isotopic signatures help identify element
origin and separate naturally occurring or background contributions from local
anthropogenicsources.Typicalsample sizes for processingare 2 liters of water, 1-10
gramsof sediment,and 1-20 gramsof soil. MeasurementlimitsforPu, Am, and Np are
< 1 X 108 atoms,and for U are < 2.5 X 1012atoms. For isotopicsignatures,< 5 X 108
atoms of Pu, Am, and Np are necessary,and 8 X 1012 atomsof U are required. Of
potential interest to the IAEA is the incorporationof these techniques into their
SafeguardsAnalyticalLaboratoryfor environmentalsampling.Studiesmadeof surface
waters,sedimentsand soilsfrom the RockyFlats Plant (RFP) in Colorado, USA, are
used as examples of this methodology. These studies showedthat, althoughplant
boundaryactinide concentrationsapproached,on the downstreamside, natural or
backgroundlevels, isotopic signaturescharacteristicof plant operations were still
discernible.
1. INTRODUCTION
The United States underground nuclear weapons test program promoted the
developmentof "clean" chemicaland instrumentalmeasurementtechniques. These
techniquespermitthe analysisofvery smallconcentrationsof actinidesextractedfrom
very complexmatrices. In supportof thismission,LosAlamosNationalLaboratorybuilt

Citations
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Journal Article•DOI•
TL;DR: A quantitative procedure for measuring subpicogram quantities of plutonium and technetium in gram quantities of geologic matrices such as uranium ores is developed, which takes advantage of the aggressive properties of sodium peroxide/hydroxide fusion to ensure complete dissolution and homogenization of complex materials.
Abstract: In uncontaminated natural materials, plutonium and technetium exist exclusively as products (daughters) of nuclear reactions in which uranium is the principal reactant (parent). Under conditions of chemical stability over geologic periods of time, the relative abundances of daughter and parent elements are fixed by the rates of nuclear reactions and the decay of the daughter radionuclide. The state of this nuclear secular equilibrium condition is the primary basis of the geochemical study of these elements in nature. Thus, it is critical that nuclear parent and daughter abundances are measured in the same sample. We have developed a quantitative procedure for measuring subpicogram quantities of plutonium and technetium in gram quantities of geologic matrices such as uranium ores. The procedure takes advantage of the aggressive properties of sodium peroxide/hydroxide fusion to ensure complete dissolution and homogenization of complex materials, the precision provided by isotope dilution techniques, and the...

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TL;DR: In this article, the incompleteness of the abstract of the paper is addressed. But the abstract is incomplete and cannot be found in the full version of this paper. citation downloaded from http://cdsweb. cern. ch/search. py?recid=452744&ln=en on 20041019
Abstract: We apologize for the incompleteness of the abstract. Citation downloaded from http://cdsweb. cern. ch/search. py?recid=452744&ln=en on 20041019

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