CArbon-14 Source Term CAST

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Presentation transcript:

CArbon-14 Source Term CAST CAST Symposium - Outcome Work Package 4 14C in Spent Ion Exchange Resins (SIERs) Name: Pascal E. Reiller Date: 17/01/2018 (Lyon) The project has received funding from the European Union’s European Atomic Energy Community’s (Euratom) Seventh Framework Programme FP7/2007-2013 under grant agreement no. 604779, the CAST project.

Why? Ion Exchange Resins (IERs) Spent Ion Exchange Resins Used for the purification of liquid processes or waste streams Water clean-up systems in the reactor coolant Spent Ion Exchange Resins IERs which were discharged from reactor, considered as carrying 14C In facilities everything is mixed PWR

Why? 14C Forms Polystyrene divinylbenzene copolymer Highly linked with the chemical conditions of the reactor BWR (oxidizing) PWR (reducing) Polystyrene divinylbenzene copolymer Cation Exchange Resin Sulphonated 13C, 17O Anionic Resin Quaternary trimethylamine 14N, 13C, 17O

Why? Thermodynamic p.o.v. 14C forms Only C1 component are stable Alcohol, aldehydes, acids are metastable 14C forms Ionisable species (carboxylic acid…) were awaited to be retained on SIERs

Why? What has been observed before CAST? Data are scarce and difficult to be made generic Magnusson & Stenström, SKB R-05-78 (2005) Park et al., J. Radioanal. Nucl. Chem. 277, 503 (2008) Vaitkevičiene et al., Radiocarbon 55, 783 (2013)

Why? If 14C is in CO32- or carboxylate form If SIERs in cement media Resins “regeneration” by OH- It is possible to immobilize SIERs in cement Pointeau et al., Radiochim. Acta 96, 367 (2008)

WP 4 Overview Objectives 7 contributions The aim of WP4 is to obtain a better understanding of the 14C source term from Spent Ion Exchange Resins of different origins (BWR or PWR) and under different storage strategies and likely release and chemical species under geological disposal conditions. This will be achieved by reviewing the current status of understanding, characterising the 14C inventory and its speciation and undertaking experiments to measure 14C release to gas and solution and its speciation 7 contributions 6 countries 7 partners Czech Republic ÚJV Řež (P. Večernik) France CEA (J. Comte, D. Lebeau, S. Legand) EDF (G. Heisbourg, L. Petit) Germany FZJ (C. Rizzato, W. von Lenza, N. Shcherbina) Italy ENEA (A. Rizzo) Romania RATEN-ICN (C. Bucur) Sweden SKB (K. Källström)

Organisation 4 TASKS Task 4.1: Current status review of 14C and its release from SIERs CEA/All D4.1: Rizzato et al. (2014) http://www.projectcast.eu/cms-file/get/iFileId/2503 Task 4.2: 14C Inventory and speciation in SIERs BWR (FZJ/SKB) PWR (CEA-EdF/SKB/ RATEN ICR/ENEA) D4.2: Reiller et al. (2014) http://www.projectcast.eu/cms-file/get/iFileId/2492 D4.3: Bucur et al. (2015) http://www.projectcast.eu/cms-file/get/iFileId/2513 D4.4: Comte et al. (2017) http://www.projectcast.eu/cms-file/get/iFileId/2548 D4.5: Rizzo et al. (2017) http://www.projectcast.eu/cms-file/get/iFileId/2587 Task 4.3: 14C release from SIERs and its speciation RATEN ICR/CEA/FZJ/ÚJV D4.3: Bucur et al. (2015) http://www.projectcast.eu/cms-file/get/iFileId/2513 D4.4: Comte et al. (2017) http://www.projectcast.eu/cms-file/get/iFileId/2548 D4.7: Bucur et al. (2017) http://www.projectcast.eu/cms-file/get/iFileId/2584 Task 4.4: Synthesis of experimental data and interpretation – final report CEA-FZJ/All D4.8: Rizzato et al. (2017) http://www.projectcast.eu/cms-file/get/iFileId/2589

TASKS OUTCOME Choice of the Samples Rizzato C., Rizzo A., Heisbourg G., Večerník P., Bucur C., Comte J., Lebeau D. & Reiller, P. E. 2014. State of the Art Review on Sample Choice, Analytical Techniques and Current Knowledge of Release from Spent Ion-Exchange Resins (D4.1). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.1. http://www.projectcast.eu/cms-file/get/iFileId/2503. Cross section of a “Mercure” C1PG package (SOCODEI) Samples CEA-EDF: PWR ENEA: PWR FZJ: BWR RATEN-ICN: CANDU SKB: PWR & BWR UJV: PWR & Research reactor Samples cannot be considered as the final waste forms

TASKS OUTCOME Annual Reports Reiller P. E., Bucur C., Comte J., Heisbourg G., Lebeau D., Rizzato C., Rizzo A. & Večerník, P. 2014. Annual Progress Report on WP4 – 2014 – (D4.2). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.2. http://www.projectcast.eu/cms-file/get/iFileId/2492. Bucur C., Comte, J., Legand, S., Rizzato, C., RIZZO, A., Večerník, P. & REILLER, P. E. 2015. 2nd Annual Progress Report on WP4 – 2015 – (D4.3). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.3. http://www.projectcast.eu/cms-file/get/iFileId/2513 . Comte J., Bucur C., Rizzato C., Rizzo A., Källström K., Večerník P. & Reiller, P. E. 2017. 3rd Annual Progress Report on WP4 – 2016 – (D4.4). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.4. Available from http://www.projectcast.eu/cms-file/get/iFileId/2548.

TASKS OUTCOME Final Outcome Rizzo A., Bucur C., Comte J., Källström K., Rizzato C., Večerník P. & Reiller P. E. 2017. Final Report on the Estimation of the Source Term and Speciation (D4.5). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.5. http://www.projectcast.eu/cms-file/get/iFileId/2587. Večerník P., Bucur C., Bujoreanu L., Comte J., Diaconescu C., Dobrin R., Legand S., Reiller P. E., Rizzato C. & Shcherbina, N. in review. Final report on leaching and desorption experiments of 14C rom Spent Ion Exchange Resins (D4.6). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.6. Bucur C., Rizzato C. & Shcherbina N. 2017. Final Report on gaseous release of C-14 from BWR and CANDU Spent Ion Exchange Resins (D4.7). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.7. Available from http://www.projectcast.eu/cms-file/get/iFileId/2584. Rizzato C., Shcherbina N. & Reiller, P. E. 2017. Compilation and comparison of data on 14C from spent ion-exchange resins (D4.8). Carbon-14 Source Term (CAST) Project, N° 604779, CAST - D4.8. http://www.projectcast.eu/cms-file/get/iFileId/2589.

WP4 Interim Technical Meetings Paris 4th-5th June 2015 Pitesti 13th-14th June 2016 Paris 10th-11th May 2017

Performance assessment Abstraction process Real system Process-level model Performance assessment model SA abstraction: The process of developing a safety assessment model from relevant phenomenological knowledge, taking into account the limits of, and uncertainties in, this knowledge, as well as requirements that may include : the types of safety and performance indicators to be calculated, the need of conservatism : simplification without undermining safety Intentionally ignore beneficial processes that are difficult to characterise Intentionally bind detrimental processes that are difficult to characterise The ease of verification of the computer code used to implement the model.

Presentations Jérôme Comte (CEA-EDF) Crina Bucur (RATEN-ICN) C-14 Content and Speciation of SIERs from PWR Crina Bucur (RATEN-ICN) C-14 Content and Speciation of SIERs from CANDU Andrey Bukaemskiy (FZJ) C-14 Content and Speciation of SIERs from BWR Petr Večerník (ÚJV) Cementation of SIERs and Consequences on C-14 mobility Antonietta Rizzo (ENEA) Evolution of Ion Exchange Resins Klas Källström (SKB) 14C: The Need for Better Understand the Inventory for Post Closure Safety

Wrap-up Have we progressed on Organic/Inorganic?

Wrap-up Have we progressed on speciation? Mainly formic acid is detected

Wrap-up Have we progressed on release? Need at least 0.1 M Base to release 14C Immobilization in cement

Wrap-up Outlook Heavily depend on national strategies Need to better assess the analytical strategies Very complex Better understanding of the 14C bearing molecules formation in the different compartments Knowing that everything will be mixed

Thank you note… Many Thanks WP4 members British Coordination Jérôme, Solène (French accent) Laurent (EDF resins are not the final waste form) Antonietta (Greatness in your lateness) Corrado (Good idea but let’s focus on the project at hand) Crina (For the road trip back from Pitesti) Petr (sharing the road trip back & D4.6 last Friday) Klas (Not every Swedish is laughing as loud as Gunnar Buckau) British Coordination Steve (Finally accepting only 9 deliverables) Simon (For losing trace of already published deliverables) Ellie (for being Ellie) Ally (for not being Ellie)