Characterization of radioactive waste forms

European Union

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Nuclear energy and safety

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• Publié par: EUROPEAN-UNION
• Nombre de lectures: 36
• Langue: English
• Poids de l'ouvrage: 4 Mo

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Commission of the "Eönütjean Communities
Characterization of radioactive
waste forms
Progress report for 1986
Volume 1
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Commission of the European Communities
nuclear science
and technology
Characterization of radioactive
waste forms
Progress report for 1986
Volume 1
Edited by:
F.P. Glasser, C. McCulloch
University of Aberdeen
Department of Chemistry
Meston Walk
AB9 2UE Old Aberdeen
Scotland
Work performed as part of the shared cost programme (1985-89)
on 'Management and disposal of radioactive waste'
of the European Communities
PARI [%'-?. Bib'ioiH
Directorate-General
Science, Research and Development N.C./EUK
1988 !CL' EUR 11354 EN/ Published by the
COMMISSION OF THE EUROPEAN COMMUNITIES
Directorate-General
Telecommunications, Information Industries and Innovation
Bâtiment Jean Monnet
LUXEMBOURG
LEGAL NOTICE
Neither the Commission of the European Communities nor any person acting on
behalf of then is responsible for the use which might be made of the
following information
Volume 2 ISBN 92-825-8397-X
Volumes 1 + 2 ISBN 92-825-8398-8
Cataloguing data can be found at the end of this publication
Luxembourg: Office for Official Publications of the European Communities, 1988
ISBN 92-825-8396-1 Catalogue number: CD-NA-11354-EN-C
© ECSC-EEC-EAEC, Brussels • Luxembourg, 1988
Printed in Belgium CONTENTS
1. INTRODUCTION PAGE NO.
1.1. - List of participants 1
1.2. - List of contributors 2 :
1.3. - Summary of National Pragrammes 3
1.4. - Abbreviations and Symbols g
2. MECHANISMS AND INTERACTION PHENOMENA INFLUENCING RELEASE
IN LOW AND MEDIUM LEVEL VASTE DISPOSAL SYSTEMS (RISØ) 8
2.1. - Diffusive transport from cemented waste (RMA8) through
porous barriers of clay or concrete. 8
2.2. - Leaching compared with diffusion through slabs of
concrete. H
2.3. - Results from leaching and diffusion studies. 13
2.4. - Diffusion through bitumen membranes. 20
2.5. - Results and conclusions.5
3. VASTE CHARACTERISATION 27
3.1. - Leach studies and Lysimeter data (Saclay and Grenoble) 2Ţ
3.1.1. - Full scale leach tests. 27
3.1.2. - Lysimeter.29
3.1.3. - Scale effects29
3.1.4. - Leaching fromwastesembeddedin bitumen30
3.1.5. - g fromsdin polymer31
3.2. - Activity characterisationinwastes.(Cadarache)31
3.3. - Leaching kinetics. (Demokritos) 32
3.3.1. - Experimentalprocedure32
3.3.2. - lresults33
3..4. - Formulation of a theoreticalmodelforthe elution of36
soluble salts from polymermatrices.(Demokritos)
III PAGE NO.
4. NUCLIDE CHEMISTRY IN MATRICES AND LEACHATES 42
4.1. - Speciation of the transuraniumelementsstemming from low
intermediate and high activity wastes.(Saclay)42
4.2. - Iodine in cement based matrices. (Aberdeen)44
4.2.1. - Precipitation and encapsulation 44
"4.2.2. - Iodine in OPC and BFS-OPCsystem45
4.3. - Behaviour of uranium in cementmatrices.(Aberdeen) 46
4.4. - Kinetics of activity release and equilibrium
concentrations of radionuclides. (Karlsruhe) 47
4.4.1. - Kinetics of activity release from cemented
wastes 47
4.4.2.-Investigations to determine theequilibrium
concentrations of actinides 50
5. COLLOIDSRELATEDTOLOVLEVELANDINTERMEDIATE
LEVELVASTE(Harwell)52
5.1. - Studiesofcolloidsin cementleachingprocedures52
5..1.1.-Cementformulation and leaching s52
5.2. - Colloid characterisation53
5.2.1. -ultrafiltration 53
5.2.2. - Dynamiclightscatteriung53
5.2.3. - Electrophoreticlightscattering57
5.2.4. - Scanningelectronmicroscopy61
5.2.5. - EnergydispersiveX-ray analysis6l
5.3. - Conclusions and future work 65
6. BLENDED CEMENT MATRICES (Aberdeen) 67
6.1. - The kinetics of blast furnaceslag67
6.2. - The stable phase compositionofblendedcements 72
6.2.1. - The calcium zeolitesŢ2
6.2.2. - The chemicallycomplexzeolites75
6.2.3. - Synthesis data 77
6.2.4. - Discussion77
6.3. - Veathering ofslag79
IV PAGE NO.
7. THE STABILITY OF VASTE FORMS 8l
7.1. - Physico-chemical characterisation of bitumenised
Eurochemic medium level waste. (SCK-CEN-MOL) 8
7.1.1. - The effect of specimen size
7.1.2. - Thet of pressure2
7.1.3. - Ageing behaviour3
7.2. - Ageing of embedded wastes in polymers (Grenoble)
7.3. - Cemented ion exchange resins, EMA 3 (RISØ) 8k
7.3.1. - Experimental work 85
7.4. - Vater chemistry in cement containing systems (RISØ) 86
7.4.1. - Hydroscopic properties or concrete and
cemented waste7
7.4.2. - Self healing of cracks or macropores in
concrete
7.5. - SAITS Measurements. (RISØ) 92
7.5.1. - Theory of SANS
7.5.2. - Experimental3
7.5.2.1. - materials
7.5.2.2. - sample requirements
7.5.2.3. -e preparation
7.5.2.4. - sample cuvettes^
7.5.2.5. - measurements
7.5.2.6. - data treatment5
7.5.2.7. - status
8. DURABILITY ATO ENVIRONMENTAL REACTIONS OF CEMENT AID
BITUMEN MATRICES 98
8.1. - Biodegradation studies. (Cadarache and Risø) 9
8.2. - The influence of organic complexing agents upon the
mobilisation and migration of radionuclides from ILV
contained in cement and bitumen under near-field
conditions for a repository in a salt dome. (Berlin) 9
8.3. - The effect of various substances on the hydration,
strength and durabilty of cement and concrete (Aberdeen) 103
8.3.1. - The effect on hydration 10
8.3.2. - Thet on durability5
8.4. - Carbonation in repository environments.
- V PAGE NO.
9. PROPERTIES OF CEMENT MATRICES 107
9.1. - Near field modellingincementenviranmments (Harwell)107
9.1.1. - Introduction107
9.1.2. - Anexampleoftheuseof CHEQMATE 108
9.1.3. - Resultsfromthebasecaserun112
9.1.4. - Sensitivitytoapproximationsand112
empiricaldata
9.1.5. - Conclusions and discussions117
9.2. - Solubility modelling of cements: implications for
radioactive waste immobilisation. (Aberdeen) 118
9.2.1. - Introduction 118
9.2.2. - Implicationsfromthesolubilitymodel119
9.2.3. - Theeffectsofsodiumon C-S-Hmatrices
(Aberdeen/Harwell)122
10. RADIATION EFFECTSANDRADIOLYSIS126
10.1. - Introduction126
10.2. - Radiation effects of reference waste forms. (Harwell)127
10. ,2. ,1. Samples 127
10.2,,2.Polymermatrix waste forms - the effect
ofcontainment during γ-irradiation 127
10.2.Gasevolution/absorption 129,3.
10.2.,4.Cementmatrixwasteforms129
10.2.5.BFS/OPCxwasteforms131
10. 2. 6. Future work131
10.3. -Redox potential and radiationeffect131
11. QUALITY ASSURANCE OF RADIOACTIVEVASTEPACKAGES 135
11.1. - Quality checking of vitrified high levelwaste(Harwell) 135
11.1.1. - Specimens 135
11.1.2.-Themechanical apparatus 136
11.1.3.-Datacollectionandprocessing138
11.1.4.-Simulationofspecimens139
11.1.5.-X-rayabsorptiometry-measurement on active
glasssamples139
11.1.6.-Summaryand status141
11.2.- Quality checking of waste packages (BAM Berlin) 142
11.2.1. - Progress of work143
11.3. - Quality checking of waste packages (CEN Cadarache)146
11.3.1. - Work programme 148
11.3.2. - Resultsandstateofadvancement 148
- VI INTRODUCTION
1.1. List of Participants
The experimental work reported here is being carried out under the
Indirect Action Third Programme (1985-1989) of the European Atomic
Energy Community "Management of Low and Medium Level Radioactive Waste
Forms". Task No. 3. The list of participants is given alphabetically
by national designations.
Belgium - Studie Centrum voor Kernenergie (SCK) Centre d'Etude de
l'Energie Nucleaire (CEN), Mol (with the collaboration of
Belgoprocess (ex Eurochemic)).
Denmark - Risø National Laboratory, Roskilde.
France - Commissariat a l'Energie Atomique (CEA), Centre d'Etudes
Nucléaires de Cadarache, Grenoble and Saclay.
Germany - Bundesanstalt fur Materialforschung und prufung (EAM)
Berlin
- Freie Universität Berlin (FUB), Berlin.
- Kernforschungszentrum Karlsruhe GmbH (KfK), Karlsuhe.
Greece - Nuclear Research Centre Demokritos, Athinai.
United
Kingdom - UKAEA - Atomic Energy Research Establishment (AERE),
Harwell.
- University of Aberdeen, Aberdeen.
Two other laboratories are participating in the programme but because
their contracts started late in 1986 they have not yet produced reports.
These are:
Italy - ENEA - CRE - Casaccia
united
Kingdom - Taylor Voodrow Construction Ltd., Southall.
- 1 1.2. Contributors
The identification of contracts and specific individuals who have
been responsible for submissions included in this report are a follows.
- P. van Iseghem - V. Timmermans - R. Reynders - J. Claes
(SCK/CEN Mol - BELGIUM). Contract No. Fl. IV. 0094-B.
- K. Brodersen - K. Nilsson
(RISØ) - N.L. DENMARK). Contract No. Fl.IV.0089-DK.
- J.C. Nomine - Ch. Courtois - N. Longomazino - H. Vidal - M de
Tassigny - D. Stammose - C. Poletiko - A. Sass (coordination)
(CEA - Saclay - Grenoble - Cadarache - FRANCE). Contract No.
F1.1V.0095-F.
- J.F. Manrignon.
(CEA Cadarache - FRANCE). Contract No. FI.IV.003S-F.
- P. Reimers - J.