Ce and U speciation in wasteforms for thermal treatment of plutonium bearing wastes, probed by L3 edge XANES

Abstract

X-ray absorption spectroscopy was applied to understand the speciation of elements relevant to the immobilisation and disposal of radioactive plutonium bearing wastes, utilizing Ce as a Pu surrogate. Ce L3 XANES (X-ray Absorption Near Edge Structure) characterisation of a crystallised glass material produced by cold crucible plasma vitrification, at demonstration scale, evidenced incorporation as Ce3+ within the glass phase, providing an important validation of laboratory scale studies. U and Ce L3 XANES investigation of brannerite ceramics, U0.9Ce0.1Ti2O6, synthesized under oxidizing, neutral and reducing conditions, established the charge compensation mechanism as incorporation of Ce3+ through formation of U5+ and/or U6+ In each of these examples, X-ray Absorption Spectroscopy has provided a pivotal understanding of element speciation in relation to the mechanism of incorporation within the host wasteform intended for geological disposal.

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Authors/Creators:

Bailey, D.J. https://orcid.org/0000-0002-0313-8748
Stennett, M.C. https://orcid.org/0000-0002-8363-9103
Sun, S.K.
Gardner, L.J. https://orcid.org/0000-0003-3126-2583
Walling, S.A.
Corkhill, C.L. https://orcid.org/0000-0002-7488-3219
Ravel, B.
Hyatt, N.C.

© 2020 The Authors. Content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence (https://creativecommons.org/licenses/by/3.0/). Any further distribution of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.

Dates:

Published: 1 April 2020

Institution:

The University of Sheffield

Academic Units:

The University of Sheffield > Faculty of Engineering (Sheffield) > Department of Materials Science and Engineering (Sheffield)

Funding Information:

Funder	Grant number
ROYAL ACADEMY OF ENGINEERING (THE)	UNSPECIFIED
ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL	EP/M026566/1
DEPARTMENT OF ENERGY AND CLIMATE CHANGE	NONE
ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL	EP/N017374/1
ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL	RG.IPSE.109543
US DEPARTMENT OF ENERGY	UNSPECIFIED
ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL	EP/T011424/1

Depositing User:

Symplectic Sheffield

Date Deposited:

11 May 2020 08:03

Last Modified:

11 May 2020 08:03

Status:

Published

Publisher:

IOP Publishing

Refereed:

Yes

Identification Number:

https://doi.org/10.1088/1757-899x/818/1/012019

CORE (COnnecting REpositories)

Ce and U speciation in wasteforms for thermal treatment of plutonium bearing wastes, probed by L3 edge XANES

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