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Speciation and Solubility Calculations for Waste Relevant Radionuclides in Boom Clay

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Speciation and Solubility Calculations for Waste Relevant Radionuclides in Boom Clay EXTERNAL REPORT SCK•CEN-ER-198 14/Ssa/P-16 Speciation and solubility calculations for waste relevant radionuclides in Boom Clay First Full Draft Sonia Salah and Lian Wang SCK•CEN Contract: CO-90-08-2214-00, RP.W&D.0064 NIRAS/ONDRAF contract: CCHO- 2009-0940000, LTBC02-GEO-01 Radionuclide migration and retention processes in Boom Clay April, 2014 SCK•CEN RDD Boeretang 200 BE-2400 Mol Belgium EXTERNAL REPORT OF THE BELGIAN NUCLEAR RESEARCH CENTRE SCK•CEN-ER-198 14/Ssa/P-16 Speciation and solubility calculations for waste relevant radionuclides in Boom Clay First Full Draft Sonia Salah and Lian Wang SCK•CEN Contract: CO-90-08-2214-00, RP.W&D.0064 NIRAS/ONDRAF contract: CCHO- 2009-0940000, LTBC02-GEO-01 Radionuclide migration and retention processes in Boom Clay April, 2014 Status: Unclassified ISSN 1782-2335 SCK•CEN Boeretang 200 BE-2400 Mol Belgium © SCK•CEN Studiecentrum voor Kernenergie Centre d’étude de l’énergie Nucléaire Boeretang 200 BE-2400 Mol Belgium Phone +32 14 33 21 11 Fax +32 14 31 50 21 http://www.sckcen.be Contact: Knowledge Centre [email protected] COPYRIGHT RULES All property rights and copyright are reserved to SCK•CEN. In case of a contractual arrangement with SCK•CEN, the use of this information by a Third Party, or for any purpose other than for which it is intended on the basis of the contract, is not authorized. With respect to any unauthorized use, SCK•CEN makes no representation or warranty, expressed or implied, and assumes no liability as to the completeness, accuracy or usefulness of the information contained in this document, or that its use may not infringe privately owned rights. SCK•CEN, Studiecentrum voor Kernenergie/Centre d'Etude de l'Energie Nucléaire Stichting van Openbaar Nut – Fondation d'Utilité Publique ‐ Foundation of Public Utility Registered Office: Avenue Herrmann Debroux 40 – BE‐1160 BRUSSEL Operational Office: Boeretang 200 – BE‐2400 MOL Abstract The Boom Clay formation represents the reference host rock for the geological disposal of high- level and/or long-lived radioactive waste (HLW-LL) in Belgium. The Belgian authority responsible for the long-term management of radioactive waste is ONDRAF/NIRAS (Organisme National des Déchets Radioactifs et Matières Fissiles Enrichies/Nationale Instelling voor Radioactief Afval en Verrijkte Splijstoffen). The current focus of the research programme of ONDRAF/NIRAS (O/N) is the so-called Safety and Feasibility Case 1 (SFC-1), which represents a body of sound arguments and evidences describing, quantifying and substantiating that geological disposal of high-level and/or long-lived radioactive waste is a safe and feasible long- term solution. In order to calculate the release and transport of the waste relevant radionuclides (RNs) through the near-field of the repository and the host clay layer (far-field), different parameters, such as concentration/solubility limits, retardation factors, diffusion accessible porosity values and pore diffusion coefficients are needed. In this report, the solubility assessment methodology, i.e. results of the speciation calculations and derivation of the RN concentration/solubility limits applicable for "undisturbed" Boom Clay conditions (far-field) will be presented. The solubility and speciation modelling was performed with the geochemical computer code The Geochemist's Workbench (versions 8.08, 8.10 and 8.12). The reference thermodynamic database that was used for the calculations and also developed at SCK•CEN is named MOLDATA thermodynamic database (2010_MOLDATA_nov_b.dat; MOLDATA TDB, version 1). 5 Table of Contents ABSTRACT ............................................................................................................................................................. 5 TABLE OF CONTENTS ............................................................................................................................................. 6 LIST OF FIGURES .................................................................................................................................................... 8 LIST OF TABLES ...................................................................................................................................................... 9 STRUCTURE OF THE DOCUMENT .......................................................................................................................... 10 1 INTRODUCTION .......................................................................................................................................... 11 2 SYSTEM DEFINITION ................................................................................................................................... 12 2.1 THE DISPOSAL SYSTEM ........................................................................................................................................... 12 2.2 BOOM CLAY REFERENCE PORE WATER ....................................................................................................................... 12 2.3 COMPUTER CODE AND DATABASES ........................................................................................................................... 13 2.4 MOLDATA ........................................................................................................................................................ 13 2.5 GDP .................................................................................................................................................................. 14 3 SPECIATION CALCULATIONS AND POURBAIX DIAGRAMS ............................................................................ 16 3.1 SPECIES ACTIVITIES AND ACTIVITY COEFFICIENTS .......................................................................................................... 17 4 SOLUBILITY ‐ DEFINITION AND THEORETICAL BACKGROUND ....................................................................... 19 4.1 SOLUBILITY CONSTANTS.......................................................................................................................................... 19 4.2 SOLUBILITY AND SATURATION .................................................................................................................................. 20 4.2.1 Calculation procedure ............................................................................................................................ 21 4.2.2 Reasoning and approach of solid phase selection .................................................................................. 21 4.2.3 Solubility Source and Expert ranges ....................................................................................................... 23 4.2.4 Uncertainties .......................................................................................................................................... 23 4.3 PARAMETERS INFLUENCING SOLUBILITY ..................................................................................................................... 25 4.3.1 Influence of particle size ......................................................................................................................... 25 4.3.2 Ostwald rule and ripening ...................................................................................................................... 25 4.3.3 Influence of temperature and pressure .................................................................................................. 26 4.3.4 Influence of ionic strength ...................................................................................................................... 26 4.3.5 Influence of inorganic complexation ...................................................................................................... 26 4.3.6 Dissolved Organic Carbon in BC porewater ............................................................................................ 27 4.3.7 Influence of organic complexation ......................................................................................................... 28 4.3.8 Influence of colloids ................................................................................................................................ 28 4.3.9 Influence of Eh, pH and pCO2 .................................................................................................................. 30 4.3.10 Influence of radiation ........................................................................................................................ 30 4.4 THE ROLE OF SOLID SOLUTIONS ................................................................................................................................ 31 4.4.1 Drawbacks for the application of solid solution models ......................................................................... 32 5 RESULTS ..................................................................................................................................................... 33 5.1 ACTINIUM (AC) .................................................................................................................................................... 35 5.2 AMERICIUM (AM) ................................................................................................................................................. 36 5.3 BERYLLIUM (BE) ................................................................................................................................................... 41 5.4 CALCIUM (CA) ....................................................................................................................................................
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