Technical Feasibility and Evaluation Study of Modern Computational Chemistry Methods for the Study of High Atomic Number Materials
Lead Research Organisation:
University of Manchester
Department Name: Chemistry
Abstract
As defined in the case for support.
Planned Impact
As defined in the case for support.
Organisations
People |
ORCID iD |
| Nik Kaltsoyannis (Principal Investigator) |
Publications
Ofili NER
(2020)
Adsorption of U(VI) on Stoichiometric and Oxidised Mackinawite: a DFT Study.
in Environmental science & technology
Tanti J
(2021)
Computational study of the substitution of early actinides and Ce into zirconolite
in Journal of Nuclear Materials
Townsend LT
(2020)
Formation of a U(VI)-Persulfide Complex during Environmentally Relevant Sulfidation of Iron (Oxyhydr)oxides.
in Environmental science & technology
| Description | The objectives of this award were twofold: (i) to develop a computational model for the incorporation of actinides and cerium into zirconolite, a glass-ceramic material proposed as a wasteform for long-term storage of the UK's civil plutonium stockpile built up from several decades of nuclear fuel reprocessing and (ii) to study computationally the adsorption of actinyl species on the iron-sulfur mineral mackinawite, and to explore the use of the computational results for the interpretation of experimentally-acquired extended X-ray absorption fine structure spectroscopy (EXAFS) data. The objectives have been met, and we have thus far produced three research papers describing our findings, one on the zirconolite work and two on the mackinawite study. For the former, we have developed a novel embedded cluster model which allowed us to study the absorption of actinides, including plutonium, into zirconolite, and our comparative study of cerium incorporation allowed us to conclude that, in this context, the latter is an appropriate non-radioactive surrogate for plutonium in the context of experimental studies of waste immobilisation. We also developed a model for the adsorption of uranyl species onto mackinawite, establishing the best way to incorporate solvation by water, and showing very nice agreement with experimental EXAFS data. |
| Exploitation Route | We anticipate that these findings will be taken forward by the actinide modelling community, and hope that experimentalists using EXAFS to study actinide-mineral interactions will seek closer collaboration with modellers to ensure that as much information as possible can be extracted from their challenging experiments. We also hope that our finding that cerium is a good surrogate for plutonium gives confidence to those experimentalists using cerium to study spent nuclear fuel wasteforms. |
| Sectors | Energy |
| Description | Chemistry World article |
| Form Of Engagement Activity | A magazine, newsletter or online publication |
| Part Of Official Scheme? | No |
| Geographic Reach | International |
| Primary Audience | Professional Practitioners |
| Results and Impact | Article in Chemistry World magazine |
| Year(s) Of Engagement Activity | 2020 |
| URL | https://www.chemistryworld.com/news/uranium-compound-unearths-questions-on-nuclear-waste/4010995.art... |
| Description | Guardian article |
| Form Of Engagement Activity | A press release, press conference or response to a media enquiry/interview |
| Part Of Official Scheme? | No |
| Geographic Reach | International |
| Primary Audience | Public/other audiences |
| Results and Impact | Article in The Guardian newspaper. |
| Year(s) Of Engagement Activity | 2019 |
| URL | https://www.theguardian.com/environment/2019/dec/20/new-form-of-uranium-found-that-could-affect-nucl... |
| Description | Materials Chemistry Consortium meeting |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Professional Practitioners |
| Results and Impact | Actinyl adsorption on magnetite (111) |
| Year(s) Of Engagement Activity | 2018 |
| Description | Materials Chemistry Consortium meeting |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Professional Practitioners |
| Results and Impact | Actinyl adsorption on Iron Oxide surfaces |
| Year(s) Of Engagement Activity | 2017 |
| Description | Poster presentation on research |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Professional Practitioners |
| Results and Impact | Poster presentation by Ms Naomi Ofili at the Royal society of Chemistry Theoretical Chemistry Group Graduate student conference in Nottingham |
| Year(s) Of Engagement Activity | 2019 |
| Description | Poster presentation on research |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Professional Practitioners |
| Results and Impact | Poster presentation by Ms Naomi Ofili at the Materials Chemistry Consortium conference |
| Year(s) Of Engagement Activity | 2018 |
| Description | Poster presentation on research |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Professional Practitioners |
| Results and Impact | Poster presentation by Ms Naomi Ofili at the Uranium Science meeting in Bristol |
| Year(s) Of Engagement Activity | 2019 |
| Description | Theoretical chemistry group conference |
| Form Of Engagement Activity | A talk or presentation |
| Part Of Official Scheme? | No |
| Geographic Reach | National |
| Primary Audience | Professional Practitioners |
| Results and Impact | Actinyl adsorption on magnetite (111) |
| Year(s) Of Engagement Activity | 2018 |