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Immobilisation of caesium from crystalline silicotitanate by hot isostatic pressing

Chen, Tzu-Yu (2012)
Ph.D. thesis, University of Birmingham.

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Abstract

The main aim of this project was to develop a durable ceramic wasteform by HIPing Cs-exchanged crystalline silicotitanate (CST) used for nuclear waste clean-up. The sodium form (Na-CST) and niobium substituted sodium form (Na-Nb/CST) CST were hydrothermally synthesised and characterised. The synthesised CSTs and a commercial CST containing material, IONSIV®, were subjected to ion exchange studies and then the crystal phases present after HIPing were investigated. Cs-IONSIV® was thermally decomposed and converted to two major Cs-containing phases, Cs2TiNb6O18 and Cs2ZrSi6O15, and a series of other phases. Additionally the effect of metal addition on phase formation under HIP conditions was explored. The microstructure and phase assemblage of HIPed Cs-IONSIV® samples as a function of Cs content were examined using XRD, XRF, SEM and TEM/EDX.
To understand the Cs bonding environment in these Cs-containing phases, structural characterisation was undertaken using Rietveld analysis of synchrotron X-ray powder diffraction data and neutron diffraction data. The potential of these phases for hosting Cs+ and its decay product Ba2+ was also studied.
This thesis is also concerned with determining the aqueous durability of these HIPed samples by carrying out MCC-1 and PCT-B leach tests. These show very low Cs leach rates and the promise of safe long-term immobilisation of Cs from CSTs as well as suggesting these phases are more leach resistant than hollandite - the material targeted for Cs sequestration in Synroc.

Type of Work:Ph.D. thesis.
Supervisor(s):Hriljac, Joseph A.
School/Faculty:Colleges (2008 onwards) > College of Engineering & Physical Sciences
Department:School of Chemistry
Subjects:QD Chemistry
Institution:University of Birmingham
ID Code:3712
This unpublished thesis/dissertation is copyright of the author and/or third parties. The intellectual property rights of the author or third parties in respect of this work are as defined by The Copyright Designs and Patents Act 1988 or as modified by any successor legislation. Any use made of information contained in this thesis/dissertation must be in accordance with that legislation and must be properly acknowledged. Further distribution or reproduction in any format is prohibited without the permission of the copyright holder.
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