The nuclear waste inventory of the UK comprises large quantities of intermediate level wastes (ILW), which will be immobilised by encapsulation within a cementitious grout in stainless steel containers, followed by disposal in a deep engineered geological disposal facility (GDF) within a suitable geological formation. These wastes contain, in addition to radioactive elements, a heterogeneous mix of organic materials, including plastics, cellulose and rubber. Cellulosic items, such as cloth, tissue, filters, paper and wood, are considered particularly problematic, because they are known to be susceptible to degradation under alkaline conditions, forming small chain organic acids with the ability to complex metals and radionuclides. It is predicted that under alkaline conditions isosaccharinic acid (ISA) will form particularly strong complexes with Ni(II), Am(III), Eu(III), Np(IV), Th(IV), and U(IV). As a result, the presence of ISA could affect the migration behaviour of these elements, by increasing their solubility and reducing sorption, thus enhancing their mobility into the near and far field surrounding a GDF. During site operation and then after closure of a GDF, microbial communities have the potential to colonise the steep biogeochemical gradients, running from highly alkaline in the GDF ânear fieldâ to circumneutral pH conditions in the surrounding geosphere. Within these steep pH gradients microbial processes can control the fate of organic compounds, such as ISA, and have therefore been considered as an effective self-attenuating mechanism to remove ISA from the groundwater. This thesis aims to deliver a greater understanding of the microbial processes that can potentially use ISA as a carbon source and electron donor, removing it from solution, and thus having a positive impact on radionuclide mobility under GDF-relevant conditions. A microbial enrichment approach was chosen that approaches GDF-relevant conditions to explore the biodegradation of ISA. Cross-disciplinary analyses of water chemistry (pH, Eh, photospectroscopy, IC, ICP), mineralogy (ESEM, XRD, TEM, XAS) and microbiology (light microscopy, next generation sequencing) have demonstrated the ability of bacteria to degrade ISA over a wide range of biogeochemical conditions. Furthermore, key radionuclides (and their non-active analogues), including Ni(II) and U(VI), were precipitated from the groundwater system during ISA biodegradation. Moreover, in the case of uranium, microbial metabolism led to the reduction of U(VI) to U(IV), which is also less soluble. This study highlights the potential for microbial activity to help remove chelating agents from groundwaters surrounding an ILW GDF, and suggests that safety cases that do not include microbial processes may be overly conservative, over-estimating the impact of ISA on radionuclide transport.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:764526 |
| Date | January 2017 |
| Creators | Kuippers, Gina |
| Contributors | Lloyd, Jonathan |
| Publisher | University of Manchester |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | https://www.research.manchester.ac.uk/portal/en/theses/the-biodegradation-of-isosaccharinic-acid(6a3cd692-8997-4cbc-bd33-2bee7c9741b4).html |
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