Indo - UK Civil Nuclear Collaboration on Damage and Radiation Effects in Amorphous Materials (DREAM)

Lead Research Organisation: University of Sheffield
Department Name: Materials Science and Engineering

Abstract

The overarching objective of this proposal is to initiate an India-UK collaboration to lead development of understanding of radiation damage processes in nuclear waste glasses and glass composite materials. UK collaborators will contribute in two principal areas: provision of expertise in application of X-ray spectroscopy methods to radiation damaged materials and application of advanced analytical electron microscopy to glass and glass composite characterisation. Indian collaborators will bring many years of expertise in preparation and characterisation of radionuclide-containing nuclear glasses by electron spin and positron annihilation spectroscopies. This project will access world class central laboratories for materials irradiation and synchrotron radiation in the partner countries. The outcome of this collaboration will be to provide the fundamental understanding required to develop predictive models for performance of radiation damaged glasses in geological disposal facilities.The research programme will systematically investigate the potential for radiation induced phase separation and the impact of alpha-recoil damage on the structure, and speciation of redox active elements, in glass systems of relevance to nuclear waste immobilisation. Electron irradiation and ion beam implantation experiments will be performed to simulate the effects of beta- and alpha-decay, a combination of bulk spectroscopic and nano-scale chemical and imaging probes will be applied to determine the nature of point defects, phase separation and change in network polymerisation induced by different damage modes. We will also investigate the potential deleterious effects of radiation damage on glass dissolution rate through simple but informative alteration experiments. The proposed research is divided into three well defined research packages, with the following aims:Work Package 1: Radiation damage induced phase separation in model nuclear waste glassesThe aim of this WP is to develop an understanding of the mechanism of phase separation in nuclear waste glasses, under the influence of combined electron irradiation and radiogenic heating.Work Package 2: Radiation induced structural modification in model nuclear waste glassesThe aim of this WP is to develop an understanding of the effect of alpha-recoil damage on glass structure, using ion beam implantation combined with XAS and TEM.Work Package 3: Impact of radiation damage on dissolution of model nuclear waste glassesThe aim of this WP is to determine potential deleterious effects of radiation damage on glass dissolution, using internationally standardised short term experiments.

Planned Impact

The primary end users of this research may include Sellafield Ltd., the Radioactive Waste Management Directorate (RWMD), the Environment Agency, the Health & Safety Executive, and the National Nuclear Laboratory who are responsible, respectively, for HLW glass production, radioactive waste disposal, regulatory concerns, safety of storage and disposal, and the nuclear skills pipeline. The benefit to these organisations and the public, over the whole grant lifecycle, include: - New scientific understanding and data required to support parameterisation of models for extended interim storage and eventual disposal of HLW glass. - Demonstration of a methodology to asses impact of radiation damage on wasteform performance, guiding more informed use of expensive and hazardous actinide doping experiments. - Potential future reduction of the estimated 18 Bn cost of radioactive waste disposal, through more appropriate design of disposal facility led by an improved understanding and confidence in wasteform behaviour. - Enhanced protection of the UK population from the risk of radioactive migration, achieved by supporting more accurate knowledge of radiation damage on radionuclide release rate. - Improved public confidence in UK radioactive waste disposal strategy, through provision of underpinning scientific understanding and data, which are currently absent. - A highly skilled and knowledgeable scientist for potential recruitment. Our research could be of potential benefit to a wider user base of public and private sector organisations, suchin diverse fields such as radiopharmaceuticals, medical imaging, and homeland security. The benefit to these organisations is likely to be new insight into the design of improved radiation hard or sensitive materials, based on new understanding of the interaction of radiation with solid matter. A further beneficiary of the proposed research is the Department for Business, Innovation & Skills, since the proposed collaboration with BARC will highlight the success of the India-UK Civil Nuclear Collaboration, acting as a catalyst for further collaboration and future trade. The identified benefits will extend over the whole grant life cycle. It is our intention to publish outputs in the open peer reviewed literature, which will be immediately available to our primary user base during the design phase of the geological disposal facility over the next decade or more - assisting in building public confidence. A further near term benefit will be the availability of a highly skilled scientist, for employment in an industry in which there is substantial demand for high calibre scientists. Cost saving and safety benefits, which may be substantial, would be delivered on a timescale of several decades to several decades to several millenia.

Publications

10 25 50
 
Description This project focused primarily on the investigation of radiation damage in glass materials utilised for radioactive waste immobilisation in the UK and internationally.
An important outcome of research conducted within the framework of this project was a systematic study of the radiation stability of glass compositions utilised to immobilise UK higher activity wastes (McGann et al., J. Nucl. Mater., 429, 353-367, 2012). In particular, we demonstrated the stability of potential intermediate level waste glasses up to 8MGy, which is the expected lifetime acquired dose for such materials. We anticipate that these findings will be utilised in the disposability assessment for ILW glasses, should the UK adopt a thermal treatment approach for such wastes. The associated research publication received considerable media coverage and was highlighted in Materials World and Materials Today magazines.
The project also made a systematic study of ion beam radiation damage in borosilicate glasses, to simulate the recoil damage arising from alpha decay of actinides. Our planned X-ray absorption spectroscopy studies of ion beam damaged glasses proved extremely challenging, primarily due to the insensitivity of dopant ions to the induced damage (as probed by hard X-rays) and prohibitive atmospheric corrosion of such materials between ion implantation and XAS characterisation. Consequently, we shifted our focus to the investigation of iron phosphate glasses, which are more amenable to structural characterisation of radiation damage in the hard XAS regime. Using both XAS and Mossbauer spectroscopies we discovered reduction ion of Fe(III) to Fe(II) in these materials, as a result of ion beam implantation (Gandy et al., MRS Proceedings, 1757, 2015). If representative of radiation damage induced by alpha decay of actinides, this has important consequences for the long term stability of iron phosphate glasses as wasteform materials, since the aqueous durability is known to decrease with increasing Fe(II) content. We further investigated the incorporation of cesium iron phosphate glasses, for potential application as Cs-137 sealed sources in medicine, in collaboration with IGCAR. Using a combination of 57Fe Mossbauer spectroscopy / Fe- and P- K-edge X-ray absorption spectroscopy, we demonstrated the glass structure to be stable toward cesium incorporation at concentrations required for application (Joseph et al., J. Nucl. Mater., 494, 324-494, 2017).
Other notable achievements within the framework of this project include: a fundamental understanding of UO3 solubility in radioactive waste glasses (Connelly et al., J. Non-Cryst. Solids, 378, 282-289, 2013) and the crystal structure and defect chemistry of brannerite CeTi2O6 - of interest as an analogue ceramic for actinide disposition (Stennett et al., J. Solid State. Chem., 192, 172-178, 2012). The latter study is of particular significance in providing a plausible mechanism to explain the non-stoichiometry observed in brannerite mineral systems, which is ill understood.
The project succeeded in cultivating new collaborations with research scientists at Bhaba Atomic Research Centre and the Indira Gandhi Centre for Atomic Research. Inward and outward secondment of research personnel was achieved, to access unique facilities and research skills in the partner nations.
Following the end of the grant period, we have maintained strong UK - India collaboration, now facilitated but appointment of PDRA Dr Charu Dube to an academic position at the Central University of Gujarat, India. This collaboration has facilitated the secondment of a UK PhD candidate to work with Dr Dube to investigate radiation damage mechanisms in glass and glass-ceramic materials through access to ion beam irradiation facilities at IGCAR. The collaboration has facilitied continuity of our investigation of radiation damage effects in iron phosphate glasses, leading to two recent publications. This research has applied soft XANES spectroscopy at the Fe L2,3 edge (ca. 700 eV) to probe changes in Fe speciation induced by relatively low energy (750 keV Au+) ion beam implantation. This approach exploits the correspondence between the sampling depth of Fe L2,3 XANES in total electron yield mode and the ion beam damage depth (ca. 100 nm), extending our previous research to regimes where nuclear stopping power is dominant, as would be expected for actinide alpha-recoil damage. Importantly, this work has shown that in this regime ion beam induced radiation damage is effective in inducing Fe3+ to Fe2+, which must be accounted for in models of the long term evolution of such wasteforms incorporating actinide surrogates.
Exploitation Route We anticipate that our study of the gamma radiation stability of UK intermediate level waste glasses will be utilised in the disposability assessment for such waste packages, by NDA / RWM, should the UK adopt a thermal treatment approach for such wastes.
Sectors Energy

 
Description Our research findings have highlighted the need to incorporate a mechanistic understanding of the impact on glass dissolution kinetics of radiation damage induced changes in glass structure and microstructure, within the overall UK safety case for the geological disposal of radioactive wastes. This is evidenced by citation of research outcomes in the RWM Geological Disposal Science and Technology Plan May 2016 ; Task 541. Additionally, research initaited under this grant funded project has supported the optimisation of glass compositions to be applied as Cs-137 gamma irradiation sources, for medical applications. Development of an industrial process to manufacture such Cs-137 glasses is currently in progress. The bilateral, and wider multilateral, collaborations initaited by this project supported the conception and successful delivery of a "Joint ICTP/IAEA Workshop on radiation effects in nuclear waste forms and their consequences for storage and disposal", 12-16 September 2016, Miramare, Trieste, Italy. This event served to disseminate key findings from the project and subsequent research, by the team of collaborators, to an audience of international experts and early career researchers. The meeting was attended by 35 participants from 18 nations enabling valuable knowledge transfer of state of the art understanding of radiation damage effects in nuclear wasteforms within the international community. A further long lasting impact of this research is the development of highly skilled researchers and continuity of strong bilateral cllaboration. Two PDRAs working on the core research have progressed to independent academic positions, which has facilitated continuity of collaboration supported by secondment of PhD students.
Sector Energy,Environment,Government, Democracy and Justice
Impact Types Societal,Economic,Policy & public services

 
Description NIRAB membership
Geographic Reach National 
Policy Influence Type Participation in a advisory committee
Impact Membership of the Nuclear Innovation Research Advisory Board which developed a national R&D roadmap for nuclear fission and fusion sector, leading to announcement of £250M investment in 2015 autumn statement.
 
Description Written and oral evidence submitted to EPSRC Independent Review of Nuclear Fission and Fusion
Geographic Reach National 
Policy Influence Type Participation in a national consultation
 
Description A new precision cutting saw for radiological materials science
Amount £10,990 (GBP)
Organisation University of Sheffield 
Sector Academic/University
Country United Kingdom
Start 04/2016 
End 03/2017
 
Description DECC - MIDAS capital grant
Amount £800,000 (GBP)
Organisation Department of Energy and Climate Change 
Sector Public
Country United Kingdom
Start 04/2015 
End 03/2016
 
Description MIDAS Collaboratory
Amount £800,000 (GBP)
Organisation Department of Energy and Climate Change 
Sector Public
Country United Kingdom
Start 05/2015 
End 03/2016
 
Description NDA Bursary Scheme - Brannerite glass ceramics
Amount £45,000 (GBP)
Organisation Nuclear Decommissioning Authority NDA 
Sector Public
Country United Kingdom
Start 09/2017 
End 09/2021
 
Description Project GLAD - Phase II & II - Glass Leachability Assessment for Disposal
Amount £259,024 (GBP)
Organisation U.S. Department of Energy 
Sector Public
Country United States
Start 11/2015 
End 09/2019
 
Description RAEng Equipment Grant: Mossbauer Spectrometer
Amount £31,500 (GBP)
Organisation Royal Academy of Engineering 
Sector Charity/Non Profit
Country United Kingdom
Start  
End 03/2012
 
Description Thermal Treatment of Spent Ion Exchange Resins
Amount £25,010 (GBP)
Funding ID Award value is confidential 
Organisation Ministry of Defence (MOD) 
Sector Public
Country United Kingdom
Start 11/2018 
End 03/2020
 
Description UoS & Suppliers - MIDAS equipment match
Amount £335,000 (GBP)
Organisation University of Sheffield 
Sector Academic/University
Country United Kingdom
Start 04/2015 
End 03/2016
 
Title Brannerite crystal structure 
Description Crystal structure model of Ce0.975Ti2O6.95 deposited in Inorganic and Crystals Structure Database (ICSD). 
Type Of Material Database/Collection of data 
Year Produced 2014 
Provided To Others? Yes  
Impact Subsequent publication: Novel Chemical Synthesis and Characterization of CeTi2O6 Brannerite Linggen Kong, Daniel J. Gregg, Inna Karatchevtseva, Zhaoming Zhang, Mark G. Blackford, Simon C. Middleburgh, Gregory R. Lumpkin, and Gerry Triani, Inorganic Chemistry 2014 53 (13), 6761-6768 
 
Description Collaboration with ESRF XMAS and DUBBLE beamlines 
Organisation European Synchrotron Radiation Facility
Country France 
Sector Charity/Non Profit 
PI Contribution Extended application focus of beamline techniques to XAS data acquistion in the hard X-ray regime.
Collaborator Contribution Beamline optimisation to acquire XAS data from glass and ceramic materials in support of plutonium disposition.
Impact See publications section.
Start Year 2016
 
Description ELETTRA 
Organisation Elettra Sincrotrone Trieste
Country Italy 
Sector Academic/University 
PI Contribution Commissioning of electron yield detection for insulating samples.
Collaborator Contribution Assistance with optimisation of XAS experiments.
Impact No outputs to date.
Start Year 2012
 
Description HZDR SPIRIT Ion Beam Irradiation - India & DISTINCTIVE project. 
Organisation Helmholtz Association of German Research Centres
Department Helmholtz-Zentrum Dresden-Rossendorf
Country Germany 
Sector Academic/University 
PI Contribution Design of ion beam irradiation experiments
Collaborator Contribution Ion beam irradiation of samples for experimental study
Impact No output other than publication listed elsewhere on the form.
Start Year 2012
 
Description IUAC - New Delhi 
Organisation Inter University Accelerator Centre
Country India 
Sector Academic/University 
PI Contribution Design of ion beam implantation experiments and characterisation of ion implanted materials.
Collaborator Contribution Ion beam implantation of glass and ceramic materials
Impact No outputs other than publications summarised under appropriate sections.
Start Year 2014
 
Description Indira Gandhi Centre for Atomic Research (IGCAR), India - DISTINCTIVE & India project. 
Organisation Indira Gandhi Centre for Atomic Research (IGCAR)
Country India 
Sector Academic/University 
PI Contribution Design of ion beam implantation experiments for glass ceramics, characterisation of ion implanted material.
Collaborator Contribution Ion beam implantation of glass ceramic materials.
Impact No outputs yet published.
Start Year 2015
 
Description NSLS 
Organisation Brookhaven National Laboratory
Department National Synchrotron Light Source
Country United States 
Sector Public 
PI Contribution Commissioning of grazing angle XAS capability.
Collaborator Contribution Expertise in data analysis, experiment optimisation, and software enhancements.
Impact No output other than publications reported elsewhere on the form.
Start Year 2012
 
Description RRCAT - INDUS 2 
Organisation Raja Ramanna Centre for Advanced Technology (RRCAT)
Country India 
Sector Public 
PI Contribution Design of X-ray absorption experiment for characterisation of ion beam implanted materials and analysis of data.
Collaborator Contribution Access to XAS beamline.
Impact No outcomes other than publications reported under appropriate sections.
Start Year 2015
 
Description All Party Parliamentary Group on Nuclear Energy, Palace of Westminster, London, 25 November 2015. 
Form Of Engagement Activity A formal working group, expert panel or dialogue
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Policymakers/politicians
Results and Impact Invited presentation at All Party Parliamentary Group on Nuclear Energy, Palace of Westminster, London, 25 November 2015. Attended by approximately a dozen parliamentarians and other policy makers, including Energy Minister Angela Leadsom MP. Presentation sparked questions and discussion afterwards.
Year(s) Of Engagement Activity 2015
 
Description British Embassy meeting - Dehli 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Poster presentation prompted discussion and follow up email exchange.

Further discussion of research findings.
Year(s) Of Engagement Activity 2013
 
Description IAEA Summer School on Radiation Effects on Radioactive Wasteforms 
Form Of Engagement Activity A formal working group, expert panel or dialogue
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Organised Joint ICTP-IAEA Workshop on Radiation Effects in Nuclear Waste Forms and their Consequences for Storage and Disposal, 12-16 September 2016, with engagement of over 30 international researchers.
Year(s) Of Engagement Activity 2017
URL http://indico.ictp.it/event/7633/
 
Description Interview on BBC Radio Leicester 
Form Of Engagement Activity A press release, press conference or response to a media enquiry/interview
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Media (as a channel to the public)
Results and Impact Interview sparked questions from listeners.

Not aware of any additional impact.
Year(s) Of Engagement Activity 2014
 
Description Joint ICTP-IAEA Workshop on Radiation Effects in Nuclear Waste Forms and their Consequences for Storage and Disposal 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Industry/Business
Results and Impact The Workshop aimed to gain awareness on the most recent findings of research into radiation effects in nuclear waste forms and their role for waste storage and disposal. It specifically aimed to contribute to the transfer of specific knowledge to Member States towards their capacity building efforts and competence in nuclear waste immobilisation and disposal. The workshop was attended by 35 participants from 18 nation states, including experienced and early career researchers from universities, industry and government laboratories.
Year(s) Of Engagement Activity 2016
URL http://indico.ictp.it/event/7633/overview
 
Description Keeping the lights on with Nuclear Energy! An interactive exhibit at The University of Sheffield's Discovery Night, 13 March, 2015 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Public/other audiences
Results and Impact Interactive exhibit and demonstration of a model nuclear reactor and radioactivity, with poster presentations discussing project research.
Year(s) Of Engagement Activity 2015
 
Description Last Light, Lasting Memories. 
Form Of Engagement Activity A broadcast e.g. TV/radio/film/podcast (other than news/press)
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Public/other audiences
Results and Impact Contribution to oral histories project of the National Synchrotron Light Source to commemorate last shut down and decommissioning.
Year(s) Of Engagement Activity 2014
 
Description Participation in International Glass Working Group 
Form Of Engagement Activity A formal working group, expert panel or dialogue
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Participation in International Glass Working Group - dissemination of research outcomes from multiple EPSRC sponsored projects with the aim of developing a state of the art unified model for glass corrosion, relevant to radioactive waste disposal; participation in expert group designing collaborative international experiments using International Standard Glass.
Year(s) Of Engagement Activity 2017
 
Description SET for Britain 2013 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Policymakers/politicians
Results and Impact Poster sparked considerable discussion and led to invitation to participate in an interview on BBC Radio Leicester,

Correspondence with local Member of Parliament.
Year(s) Of Engagement Activity 2014
 
Description Second Symposium on Thermal Treatment: research, Development and Demonstration, Warrington, UK. 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact One day symposium on thermal treatment of radioactive wastes which also showcased project research, with attendance from industry, regulators and policy makers both national and international. Most significant impact was increased in technology application and demand for research co-ordination.
Year(s) Of Engagement Activity 2015
 
Description Thermal Treatment: research, Development and Demonstration, Warrington, UK. 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Type Of Presentation keynote/invited speaker
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Talk sparked questions and discussion afterwards.

Requests for reprints.
Year(s) Of Engagement Activity 2014
 
Description What to do with it all: a hands on look at the disposal of radioactive waste, The Mobile University. 
Form Of Engagement Activity Participation in an open day or visit at my research institution
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Public/other audiences
Results and Impact Talk sparked questions and discussion afterwards.

None.
Year(s) Of Engagement Activity 2014
 
Description Workshop on UK-India Nuclear collaboration, Oxford. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Talk sparked questions and discussion afterwards.

Talk inspired a subsequently successful EPSRC proposal.
Year(s) Of Engagement Activity 2012
 
Description Workshop on the radiation damage of nuclear wasteforms. 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Type Of Presentation workshop facilitator
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact I organised this international workshop in Sheffield, under the auspices of the project. The meeting sparked considerable debate on recent research findings.

New collaborations were established between the delegates.
Year(s) Of Engagement Activity 2012
 
Description World of pane, article in Materials World. 
Form Of Engagement Activity A magazine, newsletter or online publication
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Public/other audiences
Results and Impact Research was highlighted by a full page article in Materials World, October issue, 2012.

Requests for paper reprint.
Year(s) Of Engagement Activity 2014