Modelling the Radiolytic Corrosion of Nuclear Fuel
Lead Research Organisation:
University of Huddersfield
Department Name: Chemistry
Abstract
Nuclear energy plays an important role in providing clean sustainable energy, mitigating the risk of climate change. Despite safety concerns, growing consensus sees the long-term storage of spent nuclear fuel in deep-underground repositories.
Dissociation of water, caused by nuclear radiation, occurs when groundwater interacts with nuclear fuel. This produces reactive oxygen species that cause oxidation of the fuel, and the release of soluble species and radionuclides into the environment, posing a threat to the ecosystem.
The project will employ computer modelling to investigate the nuclear fuel - water interface, to improve our ability to predict its long-term behavior.
Dissociation of water, caused by nuclear radiation, occurs when groundwater interacts with nuclear fuel. This produces reactive oxygen species that cause oxidation of the fuel, and the release of soluble species and radionuclides into the environment, posing a threat to the ecosystem.
The project will employ computer modelling to investigate the nuclear fuel - water interface, to improve our ability to predict its long-term behavior.
Organisations
| Description | In radiolysis, surface composition is fundamental as surface species determine the speciation of the radiolytic product and as such the rate of radiolytically driven dispersal of material into the environment. In this study we use the most up-to-date setting for our Density Functional Theory (DFT) calculations on PuO2 to generate data to implement into a thermodynamic strategy to map the morphologies of PuO2 nanoparticles as a function of temperature and pressure. We predict the interaction of H2O, H2O2 and CO2 on PuO2 surfaces at a molecular level, and use this data to generate morphology phase diagrams to aid the description of the nanoparticle morphology. By predicting the effect of small molecules prevalent in the radiolysis, (H2O, H2O2 and CO2) this study informs experiments to consider not only dissolved small molecules, but also the adsorption of these small molecules to the surface. |
| Exploitation Route | 1) We use the most up-to-date setting for our DFT calculations on PuO2: we include the Hubbard parameter, relativistic contributions, spin-orbit interactions and noncollinear magnetism. This is the only way to get the simulated structure correct as experiments have derived. These settings could be used by other researchers. 2) Our thermodynamic procedure to map data generated from DFT calculation to nanoparticle morphology could easily to applied to other materials in a wide variety of contexts. |
| Sectors | Energy,Environment |
| Title | Dataset for The Energetics of Carbonated PuO2 Surfaces Affects Nanoparticle Morphology: A DFT+U Study |
| Description | The dataset includes data relating to the publication "The Energetics of Carbonated PuO2 Surfaces Affects Nanoparticle Morphology: A DFT+U Study", https://doi.org/10.1039/D0CP00021C |
| Type Of Material | Database/Collection of data |
| Year Produced | 2020 |
| Provided To Others? | Yes |
| Impact | The data was used in the publication "The Energetics of Carbonated PuO2 Surfaces Affects Nanoparticle Morphology: A DFT+U Study", https://doi.org/10.1039/D0CP00021C |
| URL | https://huddersfield.box.com/s/ahotv651gf36avkxetub96ys4gjob54q |
| Description | Oral and Poster Presentations at Conferences |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Postgraduate students |
| Results and Impact | Oral and Poster presentations have be performed at a number of national level conferences. The posters offered an excellent opportunity for networking and discussing the work with other researchers. The talks offered an excellent opportunities to present the work to other research and industrial/business audiences. These presentations are listed below in chronological order: 1) Moxon Sam, Poster Presentation, "The reliability of Potential Models on the Vibrational Properties of Actinide Oxides", Solid State Chemistry Group Meeting 2018, London, 17-18th December 2018 2) Moxon Sam, Poster Presentation, "Assessing the Reliability of Potential Models for Simulating the Vibrational Properties of Uranium Oxide", Uranium Science Conference 2019, Bristol, 21-22nd January 2019 3) Moxon Sam, Poster Presentation, "The Interaction of CO2 with surfaces of PuO2", Insights into Processes at Minerals and Materials Surfaces and Interfaces, Huddersfield, 17th June 2019 4) Moxon Sam, Poster Presentation, "The Interaction of CO2 with surfaces of PuO2", CCP5 Summer School 2019, Durham, 8-18th July 2019 5) Moxon Sam, Poster Presentation, "The Role of CO2 on PuO2 Nanoparticle Morphology: A Prediction via Ab Initio Modelling", 39TH INTERNATIONAL CONFERENCE AND CCP5 ANNUAL GENERAL MEETING 2019 ADVANCES IN SIMULATIONS AND THEORY OF MATTER, London, 16-18th September 2019 6) Moxon Sam, Oral Presentation, "Morphology of PuO2 Nanoparticles due to CO2 interaction" 39TH INTERNATIONAL CONFERENCE AND CCP5 ANNUAL GENERAL MEETING 2019 ADVANCES IN SIMULATIONS AND THEORY OF MATTER, London, 16-18th September 2019 7) Moxon Sam, Poster Presentation, "The Interaction of CO2 with PuO2 Surfaces", 39th Christmas Meeting of the RSC Solid State Chemistry Group, Liverpool, 16-17th December 2019 8) Moxon Sam, Poster Presentation, "The Interaction CO2 with PuO2 Surfaces", New Horizons in Materials Modelling 2020, York, 10th January 2020 9) Moxon Sam, Oral Presentation, "Safe storage of actinides; a challenge for the nuclear industry", New Horizons in Materials Modelling 2020, York, 10th January 2020 |
| Year(s) Of Engagement Activity | 2018,2019,2020 |