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Copyright © 2015 SCK•CEN Development of a xenon mitigation prototype Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre (SCK•CEN), Mol, Belgium Matthias Auer, Abdelhakim Gheddou, Martin Kalinowski Preparatory Commission for the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO), Vienna, Austria Dominique Moyaux, Benoît Deconninck Institute for Radioelements (IRE), Fleurus, Belgium Project financed under the EU JA-V program 1

Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

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Page 1: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Development of a xenon mitigation prototype

Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre (SCK•CEN), Mol, Belgium

Matthias Auer, Abdelhakim Gheddou, Martin Kalinowski

Preparatory Commission for the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO), Vienna, Austria

Dominique Moyaux, Benoît Deconninck

Institute for Radioelements (IRE), Fleurus, Belgium

Project financed under the EU JA-V program

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Page 2: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Introduction

l  Objective of the International Monitoring System (IMS): At least 90% detection capability within 14 days after a nuclear explosion in the atmosphere, underwater or underground for a 1 kton nuclear explosion.

l  Radioxenons are a key component of the verification of the CTBT

l  Detection capability international noble gas network (Xe) depends on: l Number and distribution of stations (30 operational actually, 40 are planned) l Minimum Detectable Concentration (< 1mBq/m3 for Xe-133) l Background level at individual stations of radioxenons from other sources

Source Radioxenon release Hospitals ≥ 5 1010 Bq/year Be and mainly Xe-131m Nuclear Power Plants ~1015 Bq/year > 150 sites (> 1000 MW) Radiopharmaceutical facilities ~0.5 – 1 1016 Bq/year All RPFs 1 kton nuclear explosion ~1016 Bq/event Xe-133 if all released

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Page 3: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Project summary

l  Aim: Develop and test a mobile pilot system for the reduction of xenon emissions (based on physical adsorption) at IRE, Fleurus

l  Project subdivided in three phases l Phase I: Selection and study of xenon adsorption materials with

emphasis on new types of Silver Zeolites l Phase II: Study of operational conditions of a xenon trap and trap

design l Phase III: Construction and testing of a mobile trap at the IRE facility

l  At this stage of the project l Phase I è Finished l Phase II è Finished l Phase III è In progress

Main results and corresponding design in this presentation

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Page 4: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Experimental set-up at SCK•CEN

Two interchangeable columns that can be -  filled with different adsorbent materials -  cooled (ice, dry ice, …) -  heated (regeneration studies)

Thermal conductivity detector (TCD)

For tests with stable Xenon

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Page 5: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Xenon adsorption materials

l  The most promising activated carbon is Nusorb GXK l  The most promising silver zeolite is Ag-ETS-10

Ag-ETS-10 highly concentrates xenon in its volume

S. M. Kuznicki et al., Xenon adsorption on Modified ETS-10, J. Phys. Chem. C, 111 (2007) 1560-1562

F (cm³/min) T (°C) P (bar) [Xe] (ppm) 400 25 1.8 1000

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Page 6: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Comparison required adsorbent volume

l  Hypotheses l Trap used in the venting system of the dissolver l The trap should operate 80 days before regeneration (decay)

l 80 days decay è ≈ 15 T1/2 Xe-133 (reduction factor ≈ 104) l No diffusion of xenon atoms in between dissolution !

l  Adsorbent volume Adsorbent Volume (cm³) RKJ 1 7390 Nusorb GXK 5170 Ag-Chabazite (10-15%) 1100 Ag-Chabazite (25-30%) 600 Ag-ETS-10 210 Ag-ETS-10 (T= 60°C) 380

~25

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Page 7: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Ag-ETS-10 – Possible issues

l  Ag-ETS-10 highly concentrates xenon l Radioxenon with high activities in operational conditions at IRE! l Degradation of materials due to the irradiation?

l No degradation after a 1 MGy irradiation l Temperature rise in the adsorption column?

l Decreasing adsorption capacity and increasing diffusion l Calculation of the temperature inside the column (T > 200 °C)

l  Possible solutions l Mixture Ag-ETS-10 with activated carbon to increase volume l Ag-Chabazite to increase volume of trap l Replacing 1 column by 2 or 4 smaller column (Vtot=Cst) l Oversize the adsorption column for equilibrium è T ↓

l AND decrease activity by adapting the working process

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Page 8: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Helium regeneration conditions

l  Helium regeneration at different temperatures l 3 hours at fixed temperature

Run 2 221 °C Run 4 136 °C Run 7 171 °C

In these conditions, optimized T is ≈

160-170 °C

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Page 9: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Design studies

l  Different options investigated to l Reduce the activity

l  Chosen option l Reduce operating time of column (20 d)

l More columns l BUT less activity

l Oversize columns l Equilibrium

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Page 10: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Working process

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Page 11: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Dimension constraints

l  2 boxes available for the system l  Dimension of one box is too small for 6 columns

l One column ≈ 100 mm l Pb shielding

è 2 independent systems l 3 columns each l Pb shielding l Gas handling system

Box Door Depth (mm) 650 / Width (mm) 650 470 Height (mm) 780 780

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Page 12: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Overview of the system

l  Limited size l Mobility (on wheels) l  Lead shielding

l Easily removed l  Adsorption columns

l Easily removed 680 mm

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Page 13: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Adsorption columns

l  3 Identical columns l Volume of each column = 500 cm³ l Optimized L/D ratio = 10 from phase II

l L = 400 mm l D = 40 mm

l Valves to isolate and remove l Holder to fix in the system l Insertion tube for temperature sensor

l Desorption l Adsorption (decay heat)

l Filters up and downstream

l  Filling of adsorption columns l Mechanical vibration

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Page 14: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Gas handling system

l Overview l  Use of 1 column l Mode in series

l 2 columns l 3 columns

è Flexibility

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Page 15: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Conclusion & Future work

l  Adsorbent materials study l Best adsorbent is Ag-ETS-10 (new sample)

l Good durability against successive regenerations l BUT highly concentrates xenon è Temperature !

l  Study of the trap design l Optimized trap geometry è L/D ≈ 10 l Optimization of the regeneration conditions

l Helium as desorption gas è Optimal T=160-170°C for 3 hours

l  Design of the prototype l Dimension constraints è Small and flexible system

l  Prototype will be tested l At SCK•CEN for initial tests l At IRE for further tests in operational conditions (radioxenon)

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Page 16: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN 16

Thank you for your attention !

Questions ?

Page 17: Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer … · 2015-10-09 · Christophe Gueibe, Jos Rutten, Johan Camps, Klaas van der Meer Belgian Nuclear Research Centre

Copyright © 2015 SCK•CEN

Copyright © 2015 - SCK�CEN

PLEASE NOTE! This presentation contains data, information and formats for dedicated use ONLY and may not be copied,

distributed or cited without the explicit permission of the SCK•CEN. If this has been obtained, please reference it as a “personal communication. By courtesy of SCK•CEN”.

SCK•CEN Studiecentrum voor Kernenergie

Centre d'Etude de l'Energie Nucléaire Belgian Nuclear Research Centre

Stichting van Openbaar Nut Fondation d'Utilité Publique Foundation of Public Utility

Registered Office: Avenue Herrmann-Debrouxlaan 40 – BE-1160 BRUSSELS

Operational Office: Boeretang 200 – BE-2400 MOL

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