REVIEW OF THE POTENTIAL SOURCES OF ORGANIC IODIDES IN A NPP CONTAINMENT DURING A SEVERE ACCIDENT AND REMAINING UNCERTAINTIES

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REVIEW OF THE POTENTIAL SOURCES OF ORGANIC IODIDES IN A NPP CONTAINMENT DURING A SEVERE ACCIDENT AND REMAINING

UNCERTAINTIES

Valerie Holler, Nagore Grijalba Marijuan, David Suhard, Alexandre Legrand, Celine Bouvier Capely

To cite this version:

Valerie Holler, Nagore Grijalba Marijuan, David Suhard, Alexandre Legrand, Celine Bouvier Capely.

REVIEW OF THE POTENTIAL SOURCES OF ORGANIC IODIDES IN A NPP CONTAINMENT DURING A SEVERE ACCIDENT AND REMAINING UNCERTAINTIES. European Review Meet- ing on Severe Accident Research, ERMSAR, Mar 2019, PRAGUE, Czech Republic. 140, pp.107127, 2019, Annals of Nuclear Energy. �10.1016/j.anucene.2019.107127�. �hal-02635611�

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Faire avancer la sûreté nucléaire

Development of a SIMS compatible internai standard spiked resin for quantitative bio-imaging of biological samples by laser ablation ICP-MS

an application to uranium contaminated kidney samples

Valérie HOLLER. Nagore GRIJALBA, David SUHARD, Alexandre LEGRAND, Céline BOUVIER-CAPELY

Institut de Radioprotection et de Sûreté Nucléaire, PSE-SANTE/SESANE/LRSI, 31 Av de la Division Leclerc BP 17, 92262 Fontenay-aux-Roses Cedex, France

Context

It would be désirable that both samples and calibrations standards could be shared by different imaging techniques. The aim of this work is to develop a sample/standard préparation methodology compatible with laser ablation and Secondary-lon Mass Spectrometry (SIMS) analyses for a complementary analysis of uranium distribution in kidney with both techniques. On the other hand, a novel approach based on internai standard doped resin was carried out in order to incorporate a more feasible IS than 13C (1). Therefore, thulium spiked pure EPON resin was synthetized and employed to embed dehydrated samples and doped kidney homogenates based on the Chemical sample préparation protocol of biological samples for SIMS analysis (2, 3). Nevertheless, the Chemical déhydration protocol was adapted to the viscous and liquid State of the homogenates. In parallel, în order to replace the use of organ homogenates for calibration standards (laborious task and required access to animal facilities), uranium spiked resin was also tested. Then, serial thin and ultra-thin sections were eut with microtome and the homogeneity of internai standard was evaluated by randomly analysing small selected areas by LA-ICP-MS and SIMS. Laser ablation conditions were optimized to achieve complété sample consumption of the tissue whilst minimizing the pénétration into the glass slide.

Experimental procedure

Sample size ~ mm up to cm

Complementary analytical techniques

Improvement:

Sample sharing

Quantification relative Sample size ~ mm

Spécifie sample prep. (déhydration + resin embedding) Indispensable condition

Given the constraints imposed by these both Systems, the préparation of LA-ICP-MS standards was adapted to the technical requirements of SIMS.

For this, the first step is the déhydration of uranium spiked kidney homogenates (see poster Nagore GRIJALBA et al.).

Test 1 = déhydration

^*

and resin embedding of uranium spiked kidney homogenates (laser ablation standards). The resin is spiked with Tm as IS.

Homogenate alîquot + acetone

Centrifugation x6 7000 rpm, 10 min

Acetone 1 mL, x4 Acetone 0,5 mL., x2

Dryîng at room T°, 48h Capsule fitting Addition of Tm spiked resin

Oven 60°C, 48h

✓s

* SIMS Chemical déhydration protocol was adapted to the physical properties of the kidney homogenates

Resin is wet

/ Non homogeneous distribution No fiat surface

Test 2 = Alternative to dehydrated kidney homogenate. The resin is spiked with Tm as IS and U as external calibrator.

238.029

Uranium

U

[Rnl 5f i6d17s2 Actinides

’enetrating Epoi

Resin PartA pENetrating Epo>

Hardener Part B

•Super Deep Pénétration

•No VOCs ,SuPER DEep PENETRAT»

•Ea9ytouse Z : 1 •NOVOCs

•Easyto use 2:1 0.5 P**

Tm Spex solution, 1000 ppm

U as uranyl nitrate powder Epon resin Resin formatting:

- Square -> LA-ICP-MS - Capsule -> SIMS

Step 1: Tm and U homogeneity by SIMS

Superposition of 3 spectra:

Virgin Resin U Resin U + Tm Resin

Oven /

60°c, ^48hy Resin is dry --- '' Suîtable for SIMS

LA-ICP-MS analysis for calibration

✓^\

./

\

Resin formatting trapeze

Ultra-thin eut

(1 nm)

SIMS analysis >

Step 2: Calibration and analysis of QC samples by LA-ICP-MS

Ablation of 10 surfaces of O.SxO.5 mm2 Energy 100%

Fréquence 75 Hz Spot 35 pm

Speed 35 pm/s

Signal U/Signal Tm

0.6000 0.5000 0.4000

0.3000

0.2000 0.1000

y = 0,6178x + 0,002 R2 = 0,9859

Resin U (20 ppm) + Tm (35 ppm): Tm is detected, homogeneus distribution (3000 eps) Virgin resin et Resin : Tm is détectable at background level (10 eps)

..**'**< ; J

o..^{.»•••***}

...î...

0.0000 0.1000 0.2000 0.3000 0.4000 0.5000 0.6000 0.7000 Conc U/Conc Tm

Conclusions

12000 10000 8000 6000

LA-ICP-MS «Liquid ICP-MS

-Q

Q.Q.

U C

° 4000 2000

0 ^I^{I -}I i I^I

Resin déposition on glass slide needs to be optimised to obtain reproducible resin thickness !

Acknowledgments

We developed an analytical methodology based on internai standard spiked resin which will allow the quantification by LA-ICP-MS the resin embedded samples used for other imaging techniques like SIMS microscopy. The advantages of this new methodology are 1) the addition of a suitable internai standard to both matrix-matched standards and biological samples without altering their original uranium distribution, 2) an appropriate sample préparation compatible with several imaging techniques (SIMS, TEM, LA), 3) ease to préparé and 4) room température storage as a solid material which would facilitate its transport. Some optimisations are still needed, in particular to control the resin thickness. This methodology will positively contribute to the collaboration among bio-imaging techniques users.

Bibliography

The authors acknowledge funding from Orano for the postdoctorai research fellow comprised in the UKCAN project.

We also would like to thank IRSN for the access to PATERSON Platform and for its excellent technical and Personal assistance.

1. D. Frick and D. Günther, Fundamental studies on the ablation behavior of carbon in LA-ICP-MS with respect to the suitability as internai standard", Journal of Analytical Atomic Spectrometry, 27,1294, 2012.

2. C. Tessier, D. Suhard et al., Uranium microdistribution in rénal cortex of rats after chronic exposure: a study by secondary ion mass spectrometry microscopy", Microscopy and Microanalysis, 18,123, 2012.

3. D. Suhard, C. Tessier et al., Intracellular uranium distribution: comparison of cryogénie fixation versus Chemical fixation methods for SIMS analysis", Microscopy Research and Technique, 81, 855, 2018.

15th International Conférence on Laser Ablation - September 8 > 13 2019 (Maui-Hawaii, USA) Valérie Holler [email protected]