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FEBEX II Project THG Laboratory Experiments

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FEBEX II Project THG Laboratory Experiments CO 0 O C O <0 CO FEBEX II Project 0 THG Laboratory c o Experiments O 0 O Q 3 Q enresa publication tecnica 09/2004 FEBEX II Project THG Laboratory Experiments Edited by: T. Missana CIEMAT enresa ENRESA Direction de Ciencia y Tecnologia Emilio Vargas n° 7 28043 Madrid - Espana Tfno.: 91 5 668 1 00 Fax: 91 5 668 169 www.enresa.es Disen o y production: TransEdit Imprime: GRAFISTAFF, S.L. ISSN: 7 734-380X D.L.M-54 7 73-2004 Diciembre de 2004 This report has been drawn up within the context of the FEBEX project. Its contents represents only the opinion of the authors, which do not necessarily coincide with those of the other participants in the said project. Authors: CIEMAT: A M3. Fernandez, M. Garcia-Gutierrez, Ni. Mingarro, l Missana, P. Rivas. CSIC: E. Caballero, F. J. Huertas, S. Garcla-Palma, C. Jimenez de Cisneros, J. Linares, M. L. Rozalen. PSI: B. Baeyens, M. H. Bradbury. VET: A Muurinen. EMPRESARIOS AGRUPAOOS: J. L. Cormenzana fable of contents Table of contents Table of contents RESUMEN..................................................................................................................... 1 ABSTRACT..................................................................................................................... 5 1. INTRODUCTION............................................................................................................ 9 2. FEBEX BENTONITE..................................................................................................... 13 3. POREWATER IN THE CLAY BARRIER.................................................................................... 19 3.1 Experimental methods for the physico-chemical charaterisation of the FEBEX bentonite and porewater analysis ......................................................................................... 21 3.1.1 Introduction ........................................................................................... 21 3.1.2 Experimental Techniques ................................................................................22 3.1.3 Solid phase characterisation ............................................................................. 24 3.2 FEBEX bentonite porewater chemistry modelling ...............................................................35 3.2.1 Introduction ........................................................................................... 35 3.2.2 Porewater chemistry calculations in FEBEX bentonite .................................................. 38 3.3 Physicochemical properties of bentonite: effect of the exchangeable cations ............................... 40 3.3.1 Introduction ........................................................................................... 40 3.3.2 Effect of the exchange complex on the bentonite hydration properties ................................. 42 3.3.3 Isotopic study of adsorption water in bentonite. A preliminary study ..................................47 3.4 Experiences obtained in previous studies with MX-80 clay.....................................................51 3.4.1 Introduction ........................................................................................... 51 3.4.2 Equipment used for squeezing of bentonite porewaters ................................................ 51 3.4.3 Analysis methods for porewaters ........................................................................ 52 3.4.4 Experiences of pore water studies ......................................................................54 3.5 Pore water obtained by squeezing as a function of the applied pressure ....................................58 3.5.1 Introduction ........................................................................................... 58 FEBEXII project. THG Laboratory Experiments 3.5.2 Hydrodynamic results .................................................................................... 58 3.5.3 Analytical results ...................................................................................... 62 4. EFFECT OF INTERLAYER CATIONS ON THE RHEOLOGICAL PROPERTIES OF BENTONITE............................... 65 4.1 Viscosity of clay suspensions ................................................................................. 61 4.2 Materials and methods ........................................................................................ 61 4.3 Results ......................................................................................................... 61 4.3.1 Fitting of the flow curves ............................................................................... II 4.3.2 Apparent viscosity.................................................................................... II 4.4 Discussion and conclusions .................................................................................... 14 5. GEOCHEMICAL PROCESSES AT THE SMECTITE-SOLUTION INTERFACE: DISSOLUTION, TRANSPORT AND PRECIPITATION..................................................................................................... 75 5.1 Introduction .................................................................................................... 77 5.2 Materials....................................................................................................... 77 5.3 Methods ....................................................................................................... 19 5.4 Results and discussion ........................................................................................ 81 6. RADIONUCLIDE SORPTION AND MIGRATION IN BENTONITE............................................................ 93 6.1 Diffusion experiments in compacted clay................................................................... 95 6. 1.1 Introduction ........................................................................................... 95 6.1.2 Materials and methods .............................................................................. 95 6.1.3 Theoretical description ............................................................................... 96 6.1.4 Experimental methods ............................................................................... 91 6.2 Batch sorption experiments in purified clay................................................................. 101 6.2.1 Experiments with FEBEX clay...................................................................... 101 6.2.2 Experiments with MX-80 clay..................................................................... ii9 1. CONCLUSIONS......................................................................................................... 125 1.1 Porewater in the clay barrier............................................................................... 126 1.2 Effect of the interlayer cations on the rheological properties of bentonite .................................... 121 1.3 Geochemical processes at the solution/bentonite interface ...................................................121 1.4 Sorption and migration in bentonite ........................................................................ 128 8. REFERENCES......................................................................................................... 131 IV Resumen Resumen Resumen Uno de los objetivos principales de la bentonita en □ Estudio de los efectos del complejo de cambio un almacenamiento de residues radiactivos es la de de la arcilla en sus propiedades reologicas; actuar como barrera geoqufmica a la migration de □ Identification y modelacion de los procesos que los radionucleidos. La capacidad de esta barrera tienen lugar en la interfase bentonita/agua; geoqufmica depende de sus propiedades superficia- determination de las constantes de solubilidad les y del entorno ffsico-qufmico generado par las in- de la esmectita y de formation de complejos teracciones agua/roca. superficiales; En el marco del proyecto FEBEX, se diseno un pro- □ Estudio de los mecanismos de adsorcion de grama de ensayos de laboratorio para entender los distintos radionucleidos en la bentonita. procesos fundamentales que tienen lugar en la ba ­ rrera de bentonita. Desde las primeras Loses del □ Estudio de la difusion de especies neutras y proyecto, estos ensayos de laboratorio ban permiti- anionicas para profundizar en los mecanismos do aislar distintos procesos y facilitar su interpreta ­ de exclusion anionica y obtener valores de po- tion, edemas de proporcionar parametros utiles rosidad accesible en funcion de la densidad de para su aplicacion en los modelos THM y THG. Los la bentonita; dates experimentales tambien ban side utiles para □ Completar la base de datos de coeficientes de validar los modelos THM y THG ya existentes. difusion para los trazadores utilizados en los En la segunda Lose del proyecto, los ensayos de la­ experimentos "in-situ" y "mock-up". boratories se centraron fundamentalmente en los as- El objetivo de este informe tecnico es el de resumir pectos relevantes que no babfan tenido un suficiente los principales resultados obtenidos durante la se ­ desarrollo en la Lose anterior. En particular, se desa- gunda Lose del proyecto FEBEX, por todos los grupos rrollaron las siguientes Ifneas de investigation: de investigation involucrados en el programa de en ­ □ Obtencion de una description Liable del agua sayos THG. El informe se estructurara en cuatro blo- de pore de la bentonita, en distintos condicio- ques principales, en los que se reunen las contribu- nes geoqufmicas; ciones de los distintos grupos. CIEMAT (Espana), PS I (Suiza), CSIC (Espana) y VTT
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