Silicate Nanoparticles for Extraction of Radionuclides (SINNER)

Lead Research Organisation: University of Sheffield
Department Name: Chemical & Biological Engineering

Abstract

The recently published 'Nuclear Industrial Strategy' (2013) describes clearly the aspirations of the UK government for both 'New Build' power stations and the life extension of existing nuclear fleet within this timeline. Nuclear energy also remains a strategic priority for South Korea with capacity planned to be increased by 59% by 2022. New approaches need to be developed to manage high level (HLW), intermediate level (ILW) and low level waste (LLW) in a sustainable way, as well as methods for dealing with unresolved legacy issues.
This project combines the talents and capabilities within South Korea and the UK to develop solids phase materials that actively target and extract radioactive metals from nuclear wastes. This material is capable of concentrating radioactive metal ions from large volumes of waste in which the problematic radioactive metal ion may be present in small quantities. As an example, rather than sending LLW straight to the Low Level Waste Repository (LLWR) in Cumbria, these solid phase materials can be utilised as a method of waste treatment removing the radioactivity of the LLW so it can be safely disposed of in a landfill. This approach will extend the operational life of the LLWR, where space is limited.

Solid phase extractants like these can be developed to selectively target and scavenge specific radioactive metals ions. This work will look at making new solid phase materials to target and remove specific radioactive metal ions, such a cobalt and strontium. This will be done by changing the groups that bind the metal ions on the surface of the silica solid phase.
Work will be carried out to determine how these solid phases, which are silica based, once loaded with radioactive metals can be directly converted into a glass or hybrid glass/ceramic, glass/polymer waste form. Experiments will then determine how this waste form, once made, performs in its ability to safely contain the radioactive material.

The solid phase extractants, once developed, have the ability to be applied to a number of different decommissioning and remediation issues, such as cleaning up legacy cooling pond sludges or decontamination of soil and ground water.

The results from this work will extend the applicability of selective extractants and their use into other areas, while at the same time broadening and cementing collaboration ties between South Korea and the UK in the development of decommissioning technology for future nuclear strategy.

Planned Impact

Completion of the SINNER research program will create a body of knowledge on the selective extraction of problematic radionuclides from waste streams. This work can be directly applied to decommissioning and remediation strategies both in the UK, South Korea and world-wide. It will also produce a set of new researchers whose skills will be vital to the continuing development of nuclear strategy in the coming decades. It is vital that the knowledge and skills created be supported, nurtured and maintained after the program has finished. It is also an obligation of this program to disseminate the results of our research to as wide an audience as possible; not only to peers, but to non-technical parties who take an interest in the nuclear field. Therefore our pathway to impact will focus on two routes: A) Academic impact, and B) Outreach and engagement.

The overriding priority of the program members will be to publish results in high impact open access journals. In addition; we will encourage our young researchers to present work at relevant meetings/workshops. We also propose to develop a website which will serve as a primary communication service for the UK and Korean groups participating in the project (vide infra). A priority of this program will be the establishment of an effective network within the UK and internationally with South Korea. 2 way knowledge exchange between Korea and the UK is vital to the cross fertilization of ideas and methods and is crucial to the development of this work through the initial TRL levels. Appointment of an advisory board will ensure that the research is closely aligned and informed by industrial needs. The development of a virtual centre of excellence focused on the development of separation techniques for the treatment of nuclear waste will allow researchers to engage multiple industries and research institutes including those outside of the nuclear industry interested in, for example, lanthanide recovery and separation.

Our outreach and engagement is driven to benefit the three main communities outside of academia, namely Industry, the Government and the Public. This will be achieved through a number of means;
Annual Seminars - where we present our research to an open audience
Themed Workshop - to disseminate knowledge on specific issues to industry and academic.
Website - providing a repository a repository and showcase for the outcomes of our research. Developed in multiple languages to disseminate our work to a global audience. The aim of the web-site;
Inform and update the researchers involved in the program
provide key findings to industry
Inform the advisory boards what the impact of the work will have on the nuclear roadmap
Development of material for incorporation into teaching (KS3-4, UG & PG levels)
Have a political impact, both in the UK and Korea and internationally
Training and Development - mentoring and developing our researchers in the skills and competencies that are required for continuing development of nuclear strategy in a world-wide market.
Public Engagement -participate in third party public engagement opportunities, including public lectures, debating forums, Science Week and getting actively involved with University based Public Engagement & Impact Teams.

Publications

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Amphlett J (2020) Impact of copper(II) on activation product removal from reactor decommissioning effluents in South Korea in Journal of Industrial and Engineering Chemistry

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Barton D (2019) Remediation of radioiodine using polyamine anion exchange resins in Journal of Industrial and Engineering Chemistry

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Pepper S (2017) Cobalt and nickel uptake by silica-based extractants in Separation Science and Technology

 
Description In comparison of the silica based extractant with Purolite S950 (aminophosphonic acid resin the silica based nano-particles have a lower loading capacity than equivalent functionalized polystyrene DVB based resin. This is predominantly down to the amount of extracting group placed on the solid support. The silica based extractants can load metals 2 to 3 times faster. Column work was carried out looking at a variety of activation products and radionuclides. We successfully tested a variety of functionalised silicates in both static and dynamic modes with succinic acid, phosphonic acid, BTBP and traizine functionalities. Uranium uptake and coordination on the BTBP and triazine based resins was studied using EXAFS beamtime at the Diamond Synchrotron.
It was possible to produce a solid waste form by a pelletisation process and heating above 1000 C. The material produced at lower temperatures of 800C and 900C did not prevent the metals from reacting with water. The materials also have an affinity for radionuclides such as strontium, uranium and thorium from solution. We successfully managed to convert the functionalised silicates into a glass waste form containing strontium at 1300 C, and the silicates containing uranium, thorium and lanthanum were successfully converted into a cement paste using type II Portland cement. Results from these experiments are still being written up and there should be a further 4 papers released to the literature within the next 12 months.
Key findings were as follows;
1. The functionalised silicate materials have lower loading capacities when compared to commercial equivalents.
2. Uptake kinetics are faster than polymeric materials and zeolites.
3. Some of the functionalities tested were negatively impacted by high ionic strengths expected with a decontamination solution.
4. Silicate materials once loaded have been successfully converted into a waste form compatible with current nuclear operations.
5. Uptake capacity can be increased developing more porous silicates which will have a greater surface area.
6. Chelating functionality can potentially overcome ionic strength effects.
Exploitation Route From a large consortium meeting at Kyungpook National University in South Korea on the 23rd-29th March 2018 a number of ideas were developed along with representatives from KAERI, Chungnam National University, UCLAN and Reading. The research work has been adapted to produce two funding proposals for South Korea Phase 2. Two collaborative proposals were submitted to EPSRC but were unsuccessful. We are currently exploring other opportunities to continue collaborating in this area
Sectors Energy

Environment

Security and Diplomacy

 
Description The findings from this work has gone a long way to establishing Prof. Taek Seung Lee and Prof. Kyung Jin Lee in the area of ion exchange materials for radionucide remediation. This work has been critical in giving our collaborators credibility in the nuclear community in South Korea.
First Year Of Impact 2019
Sector Education,Energy
Impact Types Cultural

Societal

 
Description DAWNMANTLE - Decontamination and waste minimisation strategies for and using advanced molten salt nuclear technologies
Amount £381,040 (GBP)
Funding ID EP/S033009/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 08/2019 
End 08/2023
 
Description Chungnam National University 
Organisation Chungnam National University
Department Organic and Optoelectronic Materials Laboratory
Country Korea, Republic of 
Sector Academic/University 
PI Contribution Sample materials, sharing of information and inclusion in presentations and papers produced from the collaboration.
Collaborator Contribution Currently have 2 visiting PDRAs from South Korea to see how we work in ion exchange.
Impact Workshop 18th-19th February 2016 held in Sheffield.
Start Year 2015
 
Description Collaboration with KAIST 
Organisation Korea Advanced Institute of Science and Technology (KAIST)
Country Korea, Republic of 
Sector Academic/University 
PI Contribution Spent a period of 2 weeks working in the laboratory of Prof. Sunyeol Choi at KAIST in Nuclear Quantum Engineering Department.
Collaborator Contribution Access to laboratories, ICP-OES and ICP-MS analysis, laboratory induction training - glove box operation, chemical consumables, UV-Vis analysis, inert atmosphere glove box access for experimental procedure develop and conducting experiments.
Impact Experimental results are still being processed and will probably lead to a publication.
Start Year 2018
 
Description Collaboration with the University of Manchester 
Organisation Manchester University
Country United States 
Sector Academic/University 
PI Contribution Discussion of ideas, development of funding proposals, hosting and support of research students and training.
Collaborator Contribution Access to ICP-OES, ICP-MS, solvent extraction equipment, chemical consumables, hosting and support of PhD students.
Impact Outcomes are still developing regarding a nuclear consortium between The University of Sheffield and the University of Manchester.
Start Year 2017
 
Description Reading University 
Organisation University of Reading
Department Department of Meteorology
Country United Kingdom 
Sector Academic/University 
PI Contribution The separations and nuclear chemical engineering research (SNUCER) group in the Department of Chemical and Biological Engineering at the University of Sheffield provide Reading with testing capability to understand and explore the extraction chemistry of the solid phase extractants manufactured by the Laurence Harwood group at Reading. We work to develop the extraction chemistry and expand the application of the resins to metal separations and generate the information required to scale up the metal recovery process.
Collaborator Contribution Prof. Laurence Harwood is continuing to supply solid phase extractants for application in decommissioning and remediation technology.
Impact This is currently developing into multiple research proposals and papers.
Start Year 2015
 
Description EPSRC UK-ROK Workshop 
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 This was a UK-ROK workshop presenting the phase 1 outcomes from the work and what the impacts and findings were. The aim of this was to establish parameters and partnerships for Phase 2. This sparked discussion about how to maximize outputs and benefits for both countries in the work that is carried out, especially considering a reduced budget next time around and potential reduction in free movement of participants.
Year(s) Of Engagement Activity 2018
URL https://epsrc.ukri.org/newsevents/events/ukrokcivilnuclearcollaborationworkshop
 
Description ICIE 2018- 7th International Conference on Ion Exchange, Yogyakarta, Indonesia 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Presentation on Recovery of Uranium from Acidic Chloride Media Using Succinate Ethyl Sulfide Functionalised Silica (STMS). This presentation was to around 120 academics, students and industrial experts as part of the international ion exchange conference. This sparked some interest and discussion regarding potential future collaboration with Japanese academics and industry widening the network development of the program to outside of the South Korean network.
Year(s) Of Engagement Activity 2018
URL http://icie.ugm.ac.id/2018
 
Description International Workshop in Sheffield on Solid Phase Extraction for Radionuclide Removal (SPEAR2) 
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 A workshop was carried out involving a large number of UK Universities, industrial representatives and Chungnam National University. The focus was to start building a network in the area of waste treatment using solid phase extraction. Representatives present were Purolite, Phosphonics, University of Reading, University of Liverpool, Manchester University, University of Leeds, University of Central Lancashire, University of Sheffield, Lancaster University, National Nuclear Laboratory and Sellafield Ltd.
Year(s) Of Engagement Activity 2016
 
Description International workshop in Liverpool on solid phase extractants for radionuclide removal (SPEAR2) 
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 Representatives from industry and academia in the UK presented research work along with representatives from South Korea. A second workshop was carried out involving a large number of UK Universities, industrial representatives and Chungnam National University. Representatives present were from Purolite, Phosphonics, University of Reading, University of Liverpool, Manchester University, University of Leeds, University of Central Lancashire, University of Sheffield, Lancaster University, National Nuclear Laboratory and Sellafield Ltd. Over two days cutting edge research was presented and discussed. In the final part of day 2 potential future directions were discussed between representatives.
Year(s) Of Engagement Activity 2017
 
Description Ion exchange experiment for student outreach activity based in the Diamond 
Form Of Engagement Activity Participation in an open day or visit at my research institution
Part Of Official Scheme? No
Geographic Reach Regional
Primary Audience Schools
Results and Impact Outreach session for approx. 30 Y12 students from a variety of regional school attended a school visit to the demand to experience engineering at Sheffield University. The students carried out a 1hr practical looking at ion exchange behavior for the removal of a contaminant (Cu2+) from water. The practical was designed to be open ended and the students got hands on experience of ion exchange and the work that the SNUCER team does at the University of Sheffield in the Department of Chemical and Biological Engineering.
Year(s) Of Engagement Activity 2016,2017,2018
 
Description Presentation at International Nuclear Engineering Conference 4th-5th October 2018 (IChemE) 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact A review presentation on Functionalised Silicates for the Remediation of and Immobilisation of Radionuclides: A South Korea and UK Project. This presented the current work that has been carried out in the SINNER program and presented the benefits and shortfalls of the research program. This sparked questions and interest from industrial representatives as well as academics. This provided a platform for discussion with academics regarding UK-ROK phase 2.
Year(s) Of Engagement Activity 2018
URL https://www.icheme.org/about-us/press-releases/nuclear-energy-and-sustainability-experts-to-arrive-i...
 
Description Schools outreach program - Resource recovery and ion exchange 10th, 14th, 16th and 22nd March 2017 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Schools
Results and Impact Dr. Sarah Pepper the PDRA on the SINNER program discussed ion exchange phenomenon and demonstrated IX uptake on one of her resin compounds (phenanthroline functionalised silicate) for the removal of copper. This was set in the context of environmental clean up.
Year(s) Of Engagement Activity 2017
 
Description Separation Science and Technology (SS&T) Conference (Tennesee) 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Presentation of current research to Department of Energy Representatives, National Laboratory Scientists, International Scientists, and US based Academics.
Year(s) Of Engagement Activity 2016
 
Description Workshop in South Korea art Chungnam National University 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Undergraduate students
Results and Impact Delegates from the UK side of the research program (Sheffield, Liverpool, and Reading) gave presentations on their research. Also interacted with undergraduates in the Engineering Department at Chungnam national University through tours, dinners and social interaction.
Year(s) Of Engagement Activity 2016