BIogeochemical Gradients and RADionuclide transport. BIGRAD

Lead Research Organisation: British Geological Survey
Department Name: Minerals & Waste

Abstract

Over 50+ years of nuclear power generation and weapons development, the UK has created large quantities of radioactive wastes. In terms of total volume, the largest fraction (> 90 %) of the higher activity waste is Intermediate Level Waste (ILW). ILW does not produce heat but contains long-lived radioisotopes, and so cannot be disposed of near the Earth's surface. The Government has recently decided that the UK's ILW should be disposed of underground (200 - 1000 m) in a 'Geological Disposal Facility' (GDF). The safety of a GDF depends on slowing the return of radioactivity from the GDF to Earth surface. Understanding the processes which control the movement of radioactivity out of the GDF and to the rock and beyond is therefore critical. The UK's ILW is very diverse and includes discarded nuclear fuel, the metal containers used to hold fuel, as well as sludges and organic debris produced when processing these radioactive materials. The UK has treated many of these radioactive wastes by immobilising them in cement and a substantial fraction of ILW has now been cemented and awaits disposal. Once the wastes have been placed in the GDF, the intention is to backfill the remaining space with cement. No site has been identified for UK wastes as yet, but it is expected that the site will be under the water table and therefore be wet. This means that, after the waste is emplaced, the GDF will rewet as groundwater percolates through the wastes. Over a long time (from hundreds to millions of years) the ILW and its steel containers will degrade, and the cement will react with the groundwater to make it very alkaline. This is a design feature, as very alkaline, 'rusty' conditions are expected to make most radioactive components of the ILW very insoluble. However, this alkaline water will react with the rock around the repository to form a 'chemically disturbed zone' (CDZ). Up until now, no studies have examined the chemical, physical and biological development of this CDZ and how this affects the mobility of radioactive contaminants from the GDF. We have chosen to study four long-lived radionuclides, the fission product technetium as well as uranium, neptunium and plutonium all of which will be present over the long timescales relevant to the CDZ. In this project, we will try and understand how the CDZ will evolve over thousands to millions of years, so we can predict the movement of radioactivity through it, and help assess the safety of the GDF. To do this, we need to study the chemical, physical and biological changes which occur as the CDZ develops, and the way in which these different factors interact with each other. We will use experiments to understand these processes and, based on these, we will develop computer models to predict what will happen in the future. We have divided our work programme into three parts: 1 Geosphere Evolution, where we will examine rock and mineral interactions, and how water flow within the rock is affected by chemical and microbiological changes caused by the water from the GDF; 2 Radionuclide Form, Reaction and Transport, where we will examine the chemical form and solubility of radionuclides, their interactions with microorganisms, and with rock surfaces, and the potential for microscopic particles to carry radioactivity; 3 Synthesis and Application, where we will bring all the experimental results together and design, develop and test our computer model to examine radionuclide transport in the CDZ. To ensure we link the different parts of the project effectively, we have identified two 'cross cutting themes' (CCTs) - (i) biogeochemical processes in the CDZ; and (ii) predictive modelling of the CDZ, which will tie all the different pieces of work together. Our work will provide improved understanding of the controls on contaminant mobility across the CDZ, improve confidence in the safety of geological disposal, and hence assist the UK in the crucial task of disposing of radioactive wastes.

Publications

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Description 1) The project provided the opportunity to examine long-term batch experiments on alakline porewater-rock interaction from legacy experiments that had run for more than 17 years. This time scale wa smuch greater than studied in most experimental systems. The experiments showed that whilst calcium silicate hydrates (CSH) pahses were important over the short term (<3 years) magnesium silicates and magnesium silicate hydrates were of potential importance over longer timescales in systems containing significant amounts of magnesium minerals (e.g. dolomite and chlorite), which might be anticipated to be present in many host rocks for a geological disposal facility (GDF) for radioactive waste. To date there has been little consideration given to the role magnesium silicates in buffering the chemistry of the alkaline disturbed zone around a GDF. Parallel research on natural alkaline groundwater systems (outside the BIGRAD project) has also confirmed that magnesium silicates may be of significance over long timescales.

2) BGS experiments using flow-through columns to simulate the geochenmical evolution of a cement pore fluid leaching from a cementitious GDF have shown that reaction tends to lead to sealing and reduction in permeability with the alkaline disturbed zone (ADZ). The experiments also show that the nature of the alteration products will cahnge over time. The greatest reaction occurs with more evolved calcium-rich porefluids, rather trhan the early potassium-rich cement leachate. The calcium silicate hydrate (CSH) reaction products become progressively more calcic with time. However, as the hyperal;kaline plume wanes and is displaced by background groundwater containing bicarbonate in solution, the CSH phases will progressively dissociate and release calcium, and eventually decompose to an amorphous silica product.

3) The BGS experiments have also demonstrated that the CSH alteration products can incorporate significant amounts of both potassium and aluminium. Even with the early high potassium leachate, the principal reaction products are CSH phases that incorporate potassium, rather than discrete potassium reaction products. This will need to be taken into account when modelling the geochemical evolution of the ADZ in safety assessments for a cementitious GDF.
Exploitation Route The BIGRAD project outputs, are now being used to support the development of the safety case for radioactive waste management in the UK, as detailed in the Radioactive Waste Management Limited (RWM) Science and Technology Plan. The RWM are currently undertaking a review of the implications of the BIGRAD project for the long-term safety of a geological disposal facility. The BGS experiments on alkaline porewater-rock interaction are feeding into this programme, in regard to understanding how the mineralogy and geochemistry of on the long-term evolution of the alkaline disturbed zone around a geological disposal facility will evolve, and how this will impact on the phydrogeological properties and transport properties of the rock mass.
Sectors Energy,Environment

 
Description The project has been extended until June 2015 and the impact of the research will described more fully on completion of the project. The research to date, from the long-term experiments undertaken by BGS in collaboration with partners at the University of Manchester and University of Leeds to simulate the interaction between hyperalkaline cement leachate from a cementitious repository for radioactive waste and the host rocks, have shown the following: 1) That aluminium is significantly incorporated within calcium silicate hydrate (CSH) phases rather than zeolites. 2) That over long time scales, magnesium silicate reaction products will potentially be important within the alkali disturbed zone (ADZ) around a cementitious radioactive waste repository. Although it is shown that the alkali leachate from the cement will initially produce calcium silicate hydrate reaction products, if magnesium is available then magnesium silicate hydrate phases will form rather than CSH as the pH falls over time. These phases will potentially impact on both the geochemical properties of the ADZ and the hydrogeological (porosity and permeability) of the ADZ. This will impact on, and feed into a better understanding of how the geochemical evolution of the ADZ should be considered and modelled in performance assessment of a cementitious radioactive waste repository. 2015-2016: The BIGRAD project outputs, are now being used to support the development of the safety case for radioactive waste management in the UK, as detailed in the Radioactive Waste Management Limited (RWM) Science and Technology Plan. The RWM are currently undertaking a review of the implications of the BIGRAD project for the long-term safety of a geological disposal facility. The BGS experiments on alkaline porewater-rock interaction are feeding into this programme, in regard to understanding how the mineralogy and geochemistry of on the long-term evolution of the alkaline disturbed zone around a geological disposal facility will evolve, and how this will impact on the phydrogeological properties and transport properties of the rock mass.
First Year Of Impact 2014
Sector Energy,Environment
Impact Types Societal

 
Description Invited to attend radioactive waste management industry workshop on Long-Term Cement Studies Project, managed by NAGRA (Switzerland), in Helsinki, Finland 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Public/other audiences
Results and Impact AE Milodowski attended the Long-Term Cement Studies Workshop in Helsinki, Finland 7-9 May 2014. The Workshop formed part of the Long-Term Cement Studies (LCS) Project funded by a consortium of radioactive waste management organisations, including: NAGRA (managers, Switzerland), NDA-RWMD (UK), SKB (Sweden), Posiva Oy (Finland) and JAEA (Japan). AE Milodowski was invited to present results from research on alkali-rock interaction and mineral alteration, which included research from BGS's natural analogue studies and from the experimental work undertaken by the BGS team from the BIGRAD project.



A key impact from this work is an improved understanding of the sinks for aluminium and alkali metals (principally potassium) within the alkali disturbed zone (ADZ) around potential cementitious repositories for radioactive waste disposal. Previous understanding and current thermodynamic models used in performance assessment for evaluating the long-term evolution of the ADZ predict that zeolites should form will be the main sink of aluminium. However both natural analogue observations and results from experimental studies such as BIGRAD show that zeolites are not significant alteration products but that aluminium is significantly incorporated within calcium silicate hydrate reaction products. These phases will potentially have a significant influence on the porosity and permeability, and geochemical properties of the ADZ and will be different to that expected for zeolite behaviour in this environment
Year(s) Of Engagement Activity 2014