Method development for thermal ionization mass spectrometry in the frame of a biokinetic tracer study with enriched stable isotopes of zirconium

Greiter, Matthias; Höllriegl, Vera; Oeh, Uwe

doi:10.1016/j.ijms.2011.02.013

Cited by 11 publications

(13 citation statements)

References 26 publications

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“…Determination of zirconium concentration and isotope abundance is important for different applications such as life science [1], geology [2][3][4][5][6], environment [7], forensics [8] or nuclear field [9][10][11][12][13]. In nuclear applications, zirconium is used as a construction material in nuclear reactors [14] and is a fission product: the radioactive 93 Zr isotope is produced mainly by nuclear fission of uranium-235 in nuclear fuel.…”

Section: Introductionmentioning

confidence: 99%

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Quemet

Maillard

Ruas

2015

International Journal of Mass Spectrometry

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A new Thermal Ionization Mass Spectrometer (TIMS) analytical procedure was developed to measure with high accuracy the zirconium isotope abundance and concentration without molybdenum correction in nuclear samples. A zirconium selective separation using UTEVA column was used before the TIMS measurement in order to remove all possible isobaric interferences (Mo, Y, Nb and Ru) in the solution. The separated solution was then deposited onto a filament previously outgassed for 4 hours to reduce the molybdenum traces in the filament. Then, the filament was introduced into the TIMS source and was maintained for 4 hours at a current of 5 A (ionization filament) and 1.2 A (evaporation filament) in order to eliminate all molybdenum trace present in the filament and in the sample. This methodology allowed the zirconium isotope abundance determination without using the molybdenum interference correction equation. The analytical results obtained with a natural solution after separation is in good accordance with the reference values: bias lower than 0.16 % for the 90 Zr, 91 Zr, 92 Zr and 94 Zr isotope abundance, and a bias of ~0.8 % for the minor isotope (96 Zr) were observed. This zirconium abundance determination methodology was used on three nuclear samples. Then, the calibration of a 91 Zr spike solution was performed by reverse isotope dilution using a SPEX standard zirconium solution. The zirconium concentration determination was then performed on the three nuclear samples by isotope dilution using the SPEX standard zirconium solution and the 91 Zr spike solution. The final uncertainties were estimated to be lower than 1 %.

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Section: Introductionmentioning

confidence: 99%

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Quemet

Maillard

Ruas

2015

International Journal of Mass Spectrometry

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“…The human biokinetic data was measured in a stable tracer study executed at the Helmholtz Zentrum München (HMGU) [6,25]. It includes 16 investigations of 12 healthy humans with ingestion of a investigation-specific amount of isotopically enriched stable zirconium.…”

Section: Methodsmentioning

confidence: 99%

Bayesian model selection validates a biokinetic model for zirconium processing in humans

Schmidl

Hug

et al. 2012

BMC Syst Biol

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BackgroundIn radiation protection, biokinetic models for zirconium processing are of crucial importance in dose estimation and further risk analysis for humans exposed to this radioactive substance. They provide limiting values of detrimental effects and build the basis for applications in internal dosimetry, the prediction for radioactive zirconium retention in various organs as well as retrospective dosimetry. Multi-compartmental models are the tool of choice for simulating the processing of zirconium. Although easily interpretable, determining the exact compartment structure and interaction mechanisms is generally daunting. In the context of observing the dynamics of multiple compartments, Bayesian methods provide efficient tools for model inference and selection.ResultsWe are the first to apply a Markov chain Monte Carlo approach to compute Bayes factors for the evaluation of two competing models for zirconium processing in the human body after ingestion. Based on in vivo measurements of human plasma and urine levels we were able to show that a recently published model is superior to the standard model of the International Commission on Radiological Protection. The Bayes factors were estimated by means of the numerically stable thermodynamic integration in combination with a recently developed copula-based Metropolis-Hastings sampler.ConclusionsIn contrast to the standard model the novel model predicts lower accretion of zirconium in bones. This results in lower levels of noxious doses for exposed individuals. Moreover, the Bayesian approach allows for retrospective dose assessment, including credible intervals for the initially ingested zirconium, in a significantly more reliable fashion than previously possible. All methods presented here are readily applicable to many modeling tasks in systems biology.

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“…As an example, new TIMS methods for the analysis of subnanogram quantities of the uranium fission product 95 Zr, are now allowing us to measure isotope abundances in human samples at uncertainties o5%. 86 In the field of plant biochemistry, utilising TIMS to measure natural isotopic variations in key plant nutrients at the submicrogram level (e.g. Mg, Ca, Fe, Cu, and Zn), provides a unique insight into water-rock-plant interactions as well as carbon and nutrient cycling.…”

Section: Applications In Life Sciencesmentioning

confidence: 99%

“…87 Rb decays to 87 Sr by b À decay with a half-life of about 50 Ga. 196 85 Rb is stable. Strontium has four naturally occurring stable isotopes 84 Sr, 86 Sr, 87 Sr and 88 Sr. 87 Sr is partly radiogenic due the decay of 87 Rb. As a result, the 87 Sr/ 86 Sr ratio varies depending on the initial Rb/Sr ratio and the age.…”

Section: Rb-sr Geochronologymentioning

confidence: 99%

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Thermal Ionisation Mass Spectrometry

Bürger

Vogl

Klötzli

et al. 2014

Sector Field Mass Spectrometry for Elemental and Isotopic Analysis

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The principle of TIMS is based on the formation of atom ions on a heated filament and the separation of these ions according to their mass/charge ratio in a mass spectrometer. In general, TIMS is applied for highprecision measurements of isotope ratios. In the basic design of a modern thermal ionisation source, a surface material is used in the shape of a flat ribbon filament. Usually, a solution (separated from the matrix and containing the element of interest in high concentration) is deposited in the centre of the filament as a liquid. Applying a current to the filament will evaporate and ionise the analyte deposited on the filament. In the case of a single-filament geometry, evaporation and ionisation of the analyte is accomplished with one filament, whereas in a double filament design, evaporation and ionisation is performed on two filaments placed parallel to each other. The analyte is evaporated on one filament, with ionisation occurring when the evaporated atoms strike the ionisation filament. A magnetic sector field is used as mass separator.

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Method development for thermal ionization mass spectrometry in the frame of a biokinetic tracer study with enriched stable isotopes of zirconium

Cited by 11 publications

References 26 publications

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Determination of zirconium isotope composition and concentration for nuclear sample analysis using Thermal Ionization Mass Spectrometry

Bayesian model selection validates a biokinetic model for zirconium processing in humans

Thermal Ionisation Mass Spectrometry

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