Appel, Karen

De Samber, Björn

Izmer, Andrei

Tolmachev, Sergei

Vanhaecke, Frank

Vekemans, Bart

Vergucht, Eva

Vincze, Laszlo

English

Ghent University Academic Bibliography

LA-ICP-MS Instrumentation SR Micro-XRF InstrumentationLaser Ablation Inductively Coupled Plasma Mass Spectrometry (LA-ICP-MS) is basedon the detection of positively charged ions generated via a high temperatureplasma discharge. For these experiments, a New Wave Research UP193HE ArF*Synchrotron micro-XRF experiments were performed at Beamline L of theHamburger Synchrotronstrahlungslabor (HASYLAB), part of the DeutschesElektronen-Synchrotron (DESY) located in Hamburg, Germany.U-L peaksOverlay of point measurement spectra on U hot spots (1-5).FWHM beam ≈ 17.5 μm, 100 s RT. Intense U-Lα fluorescencepeak located at 13.6 keV shows the presence of uranium.13452U distribution derived from the high resolution scanperformed on case 1060. FWHM of the beam ≈ 17.5 μm, 4 sRT, image dimensions: 100 (10 μm) x 100 (10 μm).Intensity (cts) U238U ion intensity, ablated area: 2 mm x 2 mm, 15 µmlaser beam diameter, 10 Hz laser repetition rate, 0.70J/cm² energy density, 15 µm lateral scanning speed.1 342Intensity (cps) 238U+238U ion intensity, ablated area: 1 mm x 1 mm, 8 µmlaser beam diameter, 10 Hz laser repetition rate, 0.70J/cm² energy density, 8 µm lateral scanning speed.13 42Intensity (cps) 238U+ Graph: plot of the 239Pu+ and 241Am+ion signal intensities versus time. The americium signal does notcome from extensive peak tailing ofthe plutonium signal, since the latteris much lower in intensity. Thisthereby confirms the presence of Amwithin the investigated area.Elemental Imaging of Actinides in Human Tissues Using LA-ICP-MS and SR Micro-XRFEva VERGUCHT1*, Andrei IZMER1, Björn DE SAMBER1,2, Bart VEKEMANS1, Karen APPEL2, Sergei TOLMACHEV3, Laszlo VINCZE1 and Frank VANHAECKE11. Department of Analytical Chemistry, Ghent University, Krijgslaan 281 (S12), B-9000 Ghent, Belgium2. HASYLAB at DESY, Notkestraβe 85, D-22607 Hamburg, Germany3. United States Transuranium & Uranium Registries, College of Pharmacy, Washington State University, 1845 Terminal Dr, Ste 201, Richland, WA-99354, USALA-ICP-MS resultsHotspot 238U concentration (µg/g) 238U concentration (µg/g)1 9.6 ± 0.5 26.7 ± 1.52 0.85 ± 0.04 0.32 ± 0.023 1.35 ± 0.06 1.37 ± 0.084 0.89 ± 0.04 3.0 ± 0.2IntroductionThe aim of this study was to evaluate the capabilities and limitations of two state-of-the-art highly sensitive analytical techniques for elemental imaging of the distributionof actinides in human tissues, in both a qualitative and a semi-quantitative manner: Laser Ablation Inductively Coupled Plasma Mass Spectrometry (LA-ICP-MS) andSynchrotron Radiation (SR) micro X-Ray Fluorescence (micro-XRF) spectrometry.The United States Transuranium & Uranium Registries (USTUR) studies the uptake, the translocation and the biokinetics of actinides in humans [1]. Human tissue sectionsfrom two USTUR cases (Registrants), which were occupationally exposed to certain actinides (U, Pu, Am), were investigated in this work. Both registrants passed away in2008, i.e. a long time after the exposure. Prior to analysis, the samples were embedded in paraffin and cut in thin slices using a microtome.References Corresponding Author[1] United States Transuranium and Uranium Registries.Available from: http://www.ustur.wsu.edu/AboutUs/overview.html (Last access: 7 June 2012)* Eva Vergucht, X-ray Microspectroscopy and Imaging Group, Department of Analytical Chemistry, Ghent University,Eva.Vergucht@UGent.beLaser ablation setup (LA)ICPMass analyser(MS)DetectionInterfaceSample stagePC Advantages of SR micro-XRF Non-destructive multi-element microscopic analysis High sensitivity and low relative LODs (sub-ppm) &absolute LODs (ag-fg)Experimental conditions RF power: 852 W Flow rates He: 0.5 l/min, Ar: 0.7 l/minAdvantages of LA-ICP-MS Extreme sensitivity and detection limits (ppb-ppt) Possibility to measure isotopes and isotope ratios Rapid bulk/micro-analysis of a wide variety of sampleslaser ablation unit or a GeoLas 200M 193 nmArF* ablation unit coupled to an ELEMENTXR SF-ICP-MS instrument was applied.Experimental conditions Energy: 19.5 keV Spot size: ≈ 17 µm Ambient air sample environment1Plutonium map at the position of hot spot 1.FWHM beam ≈ 17.5 μm, 1 s RT, 5 μm step size.Pu (cts) 239Pu ion intensity, ablated area: 1 mm x 1 mm, 10 µmlaser beam diameter, 10 Hz laser repetition rate, 0.64J/cm² energy density, 10 µm lateral scanning speed.Intensity (cps) 239Pu+239Pu ion intensity, ablated area: 2 mm x 2 mm, 15 µmlaser beam diameter, 10 Hz laser repetition rate, 0.66J/cm² energy density, 15 µm lateral scanning speed.Intensity (cps) 239Pu+239Pu ion intensity, ablated area: 0.5 mm x 0.4 mm, 10 µmlaser beam diameter, 10 Hz laser repetition rate, 0.70J/cm² energy density, 10 µm lateral scanning speed.Intensity (cps) 239Pu+13 42Pu distribution derived from the high resolution scanperformed on case 0407. FWHM of the beam ≈ 17.5 μm,5 s RT, image dimensions: 101 (10 μm) x 105 (10 μm).Intensity (cts) Pu4Plutonium map at the position of hot spot 4.FWHM beam ≈ 17.5 μm, 10 s RT, 5 μm step size.Pu (cts) 3Plutonium map at the position of hot spot 3.FWHM beam ≈ 17.5 μm, 1 s RT, 5 μm step size.Pu (cts) 2Plutonium map at the position of hot spot 2.FWHM beam ≈ 17.5 μm, 1 s RT, 5 μm step size.Pu (cts) SR micro-XRF resultsU concentration (µg/g) Hotspot30.38 ± 0.33 117.81 ± 0.31 231.26 ± 0.34 38.37 ± 0.29 419.34 ± 0.31 5Semi-quantitative results were obtained using a series of standards (HAP and dried gelatinedroplets) spiked with U.ConclusionsBoth advanced methodologies are able to visualise the heterogeneous distributions of U and Pu on the microscopic level. The microscopic hot spots of U and Pu can beeasily revealed on the trace element level. Only the LA-ICP-MS measurements could show the presence of Am in case 0407. Besides the actinides of interest also Zrmicroparticles and aggregates can be reported (not shown here).Results: Case 1060 Results: Case 0407 Several times exposed to uranium: a parabronchial lymph tissue (chest)LA-ICP-MS resultsSR micro-XRF resultsSemi-quantitative results Exposure to plutonium and americium: a paratracheal lymph tissue (throat)LA-ICP-MS resultsSR micro-XRF results

Elemental imaging of actinides in human tissues using LA-ICP-MS and SR micro-XRF

https://biblio.ugent.be/publication/4144408/file/4144413

Elemental imaging of actinides in human tissues using LA-ICP-MS and SR micro-XRF

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