Monazite-type Ceramics for Conditioning of Minor Actinides

153 Pages·2013·29.56 MB·English

by  Alexandre Guignard

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Monazite-type Ceramics for Conditioning of Minor Actinides:
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ISBN 978-3-89336-889-1 182 Me
Monazite-type Ceramics for Conditioning of Minor Actinides:
Structural Characterization and Properties
Von der Fakultät für Georessourcen und Materialtechnik der
Rheinisch -Westfälischen Technischen Hochschule Aachen
zur Erlangung des akademischen Grades einer
Doktorin der Ingenieurwissenschaften
genehmigte Dissertation
vorgelegt von
Dipl.-Ing. Carole Babelot
aus Karlsruhe
Berichter: Univ.-Prof. Dr. rer. nat. Dirk Bosbach
Univ.-Prof. Dr. rer. nat. Rainer Telle
Tag der mündlichen Prüfung: 19.11.2012
Diese Dissertation ist auf den Internetseiten der Hochschulbibliothek online verfügbar

Forschungszentrum Jülich GmbH
Institut für Energie- und Klimaforschung (IEK)
Nukleare Entsorgung und Reaktorsicherheit (IEK-6)
Monazite-type Ceramics for Conditioning of
Minor Actinides: Structural Characterization and
Properties
Carole Babelot
Schriften des Forschungszentrums Jülich
Reihe Energie & Umwelt / Energy & Environment Band / Volume 182
ISSN 1866-1793 ISBN 978-3-89336-889-1
Bibliographic information published by the Deutsche Nationalbibliothek.
The Deutsche Nationalbibliothek lists this publication in the Deutsche
Nationalbibliografie; detailed bibliographic data are available in the
Internet at http://dnb.d-nb.de.
Publisher and Forschungszentrum Jülich GmbH
Distributor: Zentralbibliothek
52425 Jülich
Tel: [phone]
Fax: [phone]
Email: [email protected]
www.fz-juelich.de/zb

Cover Design: Grafische Medien, Forschungszentrum Jülich GmbH
Printer: Grafische Medien, Forschungszentrum Jülich GmbH
Copyright: Forschungszentrum Jülich 2013
Schriften des Forschungszentrums Jülich
Reihe Energie & Umwelt / Energy & Environment, Band / Volume 182
D 82 (Diss., RWTH Aachen, University, 2012)
ISSN 1866-1793
ISBN 978-3-89336-889-1
Neither this book nor any part of it may be reproduced or transmitted in any form or by any
means, electronic or mechanical, including photocopying, microfilming, and recording, or by any
information storage and retrieval system, without permission in writing from the publisher.
À tous ceux qui m’ont aidée au cours de mes études supérieures,
de Strasbourg à Jülich, en passant par Limoges.

« Je sers la science et c’est ma joie. »
Basile, disciple de Léonard.

Content

Abbreviations .................................................................................................................... vii
1. Introduction ..................................................................................................................... 1
2. Background ..................................................................................................................... 7
2.1. Nuclear fuel cycle .................................................................................................... 7
2.1.1. Spent fuel .......................................................................................................... 8
2.2. Nuclear waste management strategies ..................................................................... 9
2.2.1. Partitioning and transmutation strategy ............................................................ 9
2.2.2. Partitioning and conditioning strategy ............................................................ 11
2.3. Nuclear waste forms for the P&C strategy ............................................................ 11
2.3.1. Glasses ............................................................................................................ 12
2.3.2. Ceramics ......................................................................................................... 12
2.3.2.1. Aqueous durability of ceramics ............................................................... 14
2.3.2.2. Radiation tolerance of ceramics ............................................................... 15
2.4. Lanthanides and actinides chemistry ..................................................................... 17
2.4.1. Lanthanide chemistry ...................................................................................... 17
2.4.1.1. Lanthanum chemistry ............................................................................... 20
2.4.1.2. Europium chemistry ................................................................................. 21
2.4.2. Actinide chemistry .......................................................................................... 21
2.5. Spectroscopic methods ........................................................................................... 23
2.5.1. Time resolved laser fluorescence spectroscopy .............................................. 23
2.5.1.1. Difference between fluorescence and phosphorescence .......................... 23
2.5.1.2. Elements with fluorescence ability .......................................................... 25
2.5.1.3. Fluorescence lifetime ............................................................................... 30
2.6. Monazite ................................................................................................................ 32
2.6.1. Structure, composition and occurrence ........................................................... 32
2.6.2. Monazite versus xenotime .............................................................................. 35
2.6.3. Synthesis methods ........................................................................................... 35
2.6.4. Monazite as a host phase for actinides ............................................................ 36
3. Experimental part .......................................................................................................... 39
3.1. Chemicals, methods and apparatuses ..................................................................... 39
3.1.1. Chemicals ........................................................................................................ 39
3.1.2. Synthesis of monazite-type powder ................................................................ 39
3.1.3. Pressing and sintering of REPO pellets ......................................................... 41
4
3.1.4. Physical properties of pellets .......................................................................... 41
3.1.4.1. Density measurements ............................................................................. 41
3.1.4.2. Vickers microhardness and fracture toughness ........................................ 42
3.1.5. Thermogravimetry coupled with differential scanning calorimetry ............... 43
3.1.6. Powder X-ray diffraction analysis .................................................................. 43
3.1.7. Raman spectroscopy ....................................................................................... 44
3.1.8. Scanning electron microscope ........................................................................ 44
3.1.9. Specific surface area measurements ............................................................... 45
3.1.10. Dilatometer ................................................................................................... 45
3.1.11. Inductive coupled plasma mass spectrometry ............................................... 45
i