This thesis is devoted to the investigation of passivesafety and inherent features of subcritical nucleartransmutation systems - accelerator-driven systems. The generalobjective of this research has been to improve the safetyperformance and avoid elevated coolant temperatures inworst-case scenarios like unprotected loss-of-ow accidents,loss-of-heat-sink accidents, and a combination of both theseaccident initiators. The specific topics covered are emergencydecay heat removal by reactor vessel auxiliary cooling systems,beam shut-off by a melt-rupture disc, safety aspects fromlocating heat-exchangers in the riser of a pool-type reactorsystem, and reduction of pressure resistance in the primarycircuit by employing bypass routes. The initial part of the research was focused on reactorvessel auxiliary cooling systems. It was shown that an 80 MWthPb/Bi-cooled accelerator-driven system of 8 m height and 6 mdiameter vessel can be well cooled in the case of loss-of-owaccidents in which the accelerator proton beam is not switchedoff. After a loss-of-heat-sink accident the proton beam has tobe interrupted within 40 minutes in order to avoid fast creepof the vessel. If a melt-rupture disc is included in the wallof the beam pipe, which breaks at 150 K above the normal coreoutlet temperature, the grace period until the beam has to beshut off is increased to 6 hours. For the same vessel geometry,but an operating power of 250 MWth the structural materials canstill avoid fast creep in case the proton beam is shut offimmediately. If beam shut-off is delayed, additional coolingmethods are needed to increase the heat removal. Investigationswere made on the filling of the gap between the guard and thereactor vessel with liquid metal coolant and using water spraycooling on the guard vessel surface. The second part of the thesis presents examinationsregarding an accelerator-driven system also cooled with Pb/Bibut with heat-exchangers located in the risers of the reactorvessel. For a pool type design, this approach has advantages inthe case of heat-exchanger tube failures, particularly if wateris used as the secondary uid. This is because a leakage ofwater from the secondary circuit into the Pb/Bi-cooled primarycircuit leads to upward sweeping of steam bubbles, which wouldcollect in the gas plenum. In the case of heatexchangers in thedowncomer steam bubbles may be dragged into the ADS core andadd reactivity. Bypass routes are employed to increase the owspeed in loss-of-ow events for this design. It is shown thatthe 200 MWth accelerator-driven system with heat-exchangers inthe riser copes reasonably well with both a loss-of-ow accidentwith the beam on and an unprotected loss-of-heat-sink accident.For a total-loss-of-power (station blackout) and an immediatebeam-stop the core outlet temperature peaks at 680 K. After acombined loss-of-ow and loss-of-heat-sink accident the beamshould be shut off within 4 minutes to avoid exceeding the ASMElevel D of 977 K, and within 8 minutes to avoid fast creep.Assuming the same core inlet temperature, both the reactordesign with heat-exchanger in the risers and the downcomershave similar temperature evolutions after a total-loss-ofpoweraccident. A large accelerator-driven system of 800 MWth with a 17 mtall vessel may eventually become a standard size. For thishigher power ADS, the location of the heat-exchangers hasgreater impact on the natural convection capability. This isdue to that larger heatexchangers have more inuence on thedistance between the thermal centers during a lossof- owaccident. The design with heat-exchangers in the downcomers,the long-term vessel temperature peaks at 996 K during aloss-of-ow accident with the beam on. This does not pose athreat of creep rupture for the vessel. However, the locationof the heat-exchangers in the downcomers will probably requiresecondary coolant other than water, like for example oil (fortemperatures not higher than 673 K) or Pb/Bi coolant.

Water and vapour flows from land to sea and the atmosphere are important for water resources, coastal ecosystems and climate. This thesis investigates possible methods for modelling these flows under often encountered unmonitored hydrological conditions and data limitations. Two contrasting types of drainage basin and associated data limitation/availability cases are considered: the Swedish unmonitored near-coastal catchment areas Forsmark and Simpevarp, for which detailed spatial but not much temporal variability data is available; and the much larger Aral Sea Drainage Basin (ASDB), for which spatial hydrological information is limited, while there is relatively well-known temporal change occurring in the Aral Sea itself and in the land and water use of the region over the last 50 years. The hydrologic modelling for the Forsmark and Simpevarp catchment areas showed that the relatively large focused stream flows, and the mean values and total sums of the diffuse small stream-groundwater flow fields in between the large stream flows from land to sea are largely constrained by the catchment hydrological balances and relatively robust and certain to estimate. The ASDB hydrologic modelling indicated an evapotranspiration return flow to the atmosphere from the irrigation water input on irrigated land that is much higher than previous estimates in atmospheric modelling, implying possible considerably larger than previously estimated non-local water and climate effects of the world’s irrigated areas. The more detailed groundwater-seawater dynamics modelling carried out for the coastal parts of the ASDB showed that regional topography and bathymetry largely influence coastal water fluxes during sea level lowering, with the Aral Sea shrinkage decreasing the seawater intrusion risk into the coastal groundwater considerably more for steeper than for flatter coastal topography parts of the region.

Nuclear power generation is being regarded as a solution to ever increasing demand for electricity, and concerns over global warming and climate change due to the use of fossil fuels. Although nuclear power generation is considered to be reliable, economical, clean, and safe, the wastes produced from the nuclear fuel cycle are not, and can remain hazardous for hundreds of thousands of years. An international consensus has developed over the past several decades that deep geologic disposal of low, intermediate, and high level radioactive wastes is the best option to protect the biosphere. In this thesis, both regional scale and sub-regional scale models are created to simulate groundwater flow and transport for a representative Canadian Shield setting, honouring site-specific topography and surface water features. Sub-surface characteristics and properties are derived from numerous geoscience studies. In addition, a regional scale model is developed, centred on the Bruce Nuclear Power Development (BNPD) site near Tiverton, Ontario, and located within the Michigan Basin. Ontario Power Generation (OPG) has proposed a Deep Geologic Repository (DGR) for low & intermediate level waste (L&ILW) at the BNPD site. Paleoclimate simulations using various combinations of parameters are performed for both the Canadian Shield Sub-Regional model, and the Michigan Basin Regional model. Fracture zone permeability is a very important parameter when modelling crystalline rock settings. Migration of a unit tracer representing glacial recharge water can occur to depth in fractures of high permeability. Representative rock compressibility values are necessary as compressibilities are used to calculate storage coefficients, and the one-dimensional loading efficiency; these affect the subsurface propagation of elevated pore pressures due to glacial loading at surface. Coupled density-dependent flow and transport in paleoclimate simulations affects deep flow systems and provides a measure of flow stability, as well as increasing the mean life expectancy at depth. Finally, hydromechanical coupling is a very important mechanism for reducing vertical hydraulic gradients during a glaciation event when a hydraulic boundary condition equal to the pressure at the base of an ice-sheet is applied at ground surface. Pore water velocities are reduced, thereby retarding migration of surface waters into the subsurface environment.

Nuclear power generation is being regarded as a solution to ever increasing demand for electricity, and concerns over global warming and climate change due to the use of fossil fuels. Although nuclear power generation is considered to be reliable, economical, clean, and safe, the wastes produced from the nuclear fuel cycle are not, and can remain hazardous for hundreds of thousands of years. An international consensus has developed over the past several decades that deep geologic disposal of low, intermediate, and high level radioactive wastes is the best option to protect the biosphere. In this thesis, both regional scale and sub-regional scale models are created to simulate groundwater flow and transport for a representative Canadian Shield setting, honouring site-specific topography and surface water features. Sub-surface characteristics and properties are derived from numerous geoscience studies. In addition, a regional scale model is developed, centred on the Bruce Nuclear Power Development (BNPD) site near Tiverton, Ontario, and located within the Michigan Basin. Ontario Power Generation (OPG) has proposed a Deep Geologic Repository (DGR) for low & intermediate level waste (L&ILW) at the BNPD site. Paleoclimate simulations using various combinations of parameters are performed for both the Canadian Shield Sub-Regional model, and the Michigan Basin Regional model. Fracture zone permeability is a very important parameter when modelling crystalline rock settings. Migration of a unit tracer representing glacial recharge water can occur to depth in fractures of high permeability. Representative rock compressibility values are necessary as compressibilities are used to calculate storage coefficients, and the one-dimensional loading efficiency; these affect the subsurface propagation of elevated pore pressures due to glacial loading at surface. Coupled density-dependent flow and transport in paleoclimate simulations affects deep flow systems and provides a measure of flow stability, as well as increasing the mean life expectancy at depth. Finally, hydromechanical coupling is a very important mechanism for reducing vertical hydraulic gradients during a glaciation event when a hydraulic boundary condition equal to the pressure at the base of an ice-sheet is applied at ground surface. Pore water velocities are reduced, thereby retarding migration of surface waters into the subsurface environment.

<p>This thesis is devoted to the investigation of passivesafety and inherent features of subcritical nucleartransmutation systems - accelerator-driven systems. The generalobjective of this research has been to improve the safetyperformance and avoid elevated coolant temperatures inworst-case scenarios like unprotected loss-of-ow accidents,loss-of-heat-sink accidents, and a combination of both theseaccident initiators. The specific topics covered are emergencydecay heat removal by reactor vessel auxiliary cooling systems,beam shut-off by a melt-rupture disc, safety aspects fromlocating heat-exchangers in the riser of a pool-type reactorsystem, and reduction of pressure resistance in the primarycircuit by employing bypass routes.</p><p>The initial part of the research was focused on reactorvessel auxiliary cooling systems. It was shown that an 80 MWthPb/Bi-cooled accelerator-driven system of 8 m height and 6 mdiameter vessel can be well cooled in the case of loss-of-owaccidents in which the accelerator proton beam is not switchedoff. After a loss-of-heat-sink accident the proton beam has tobe interrupted within 40 minutes in order to avoid fast creepof the vessel. If a melt-rupture disc is included in the wallof the beam pipe, which breaks at 150 K above the normal coreoutlet temperature, the grace period until the beam has to beshut off is increased to 6 hours. For the same vessel geometry,but an operating power of 250 MWth the structural materials canstill avoid fast creep in case the proton beam is shut offimmediately. If beam shut-off is delayed, additional coolingmethods are needed to increase the heat removal. Investigationswere made on the filling of the gap between the guard and thereactor vessel with liquid metal coolant and using water spraycooling on the guard vessel surface.</p><p>The second part of the thesis presents examinationsregarding an accelerator-driven system also cooled with Pb/Bibut with heat-exchangers located in the risers of the reactorvessel. For a pool type design, this approach has advantages inthe case of heat-exchanger tube failures, particularly if wateris used as the secondary uid. This is because a leakage ofwater from the secondary circuit into the Pb/Bi-cooled primarycircuit leads to upward sweeping of steam bubbles, which wouldcollect in the gas plenum. In the case of heatexchangers in thedowncomer steam bubbles may be dragged into the ADS core andadd reactivity. Bypass routes are employed to increase the owspeed in loss-of-ow events for this design. It is shown thatthe 200 MWth accelerator-driven system with heat-exchangers inthe riser copes reasonably well with both a loss-of-ow accidentwith the beam on and an unprotected loss-of-heat-sink accident.For a total-loss-of-power (station blackout) and an immediatebeam-stop the core outlet temperature peaks at 680 K. After acombined loss-of-ow and loss-of-heat-sink accident the beamshould be shut off within 4 minutes to avoid exceeding the ASMElevel D of 977 K, and within 8 minutes to avoid fast creep.Assuming the same core inlet temperature, both the reactordesign with heat-exchanger in the risers and the downcomershave similar temperature evolutions after a total-loss-ofpoweraccident.</p><p>A large accelerator-driven system of 800 MWth with a 17 mtall vessel may eventually become a standard size. For thishigher power ADS, the location of the heat-exchangers hasgreater impact on the natural convection capability. This isdue to that larger heatexchangers have more inuence on thedistance between the thermal centers during a lossof- owaccident. The design with heat-exchangers in the downcomers,the long-term vessel temperature peaks at 996 K during aloss-of-ow accident with the beam on. This does not pose athreat of creep rupture for the vessel. However, the locationof the heat-exchangers in the downcomers will probably requiresecondary coolant other than water, like for example oil (fortemperatures not higher than 673 K) or Pb/Bi coolant.</p>

Flow instabilities occur at all scales in planetary systems. In this thesis we examine three cases of such instabilities, on three very different length scales. In the first part, we test the idea that Archean granite-greenstone belts (GGBs) form by crustal diapirism, or Rayleigh-Taylor instabilities. GGBs are characterized by large granitic domes (50-100 km in diameter) embedded in narrow keel-shaped greenstones. They are ubiquitous in Archean (> 2.5 Ga) terrains, but rare thereafter. We performed finite element calculations for a visco-elastic, temperature-dependent, non-Newtonian crust under conditions appropriate for the Archean, which show that dense low-viscosity volcanics overlying a felsic basement will overturn diapirically in as little as 10 Ma, displacing as much as 60 % of the volcanics to the lower crust. This surprisingly fast overturn rate suggests that diapiric overturn dominated crustal tectonics in the hot conditions of the Early Earth, becoming less important as the Earth cooled. Moreover, the deposition of large volumes of wet basaltic volcanics to the lower crust may provide the source for the formation of the distinctly Archean granitic rocks which dominate Earth's oldest continents. The second part examines the origin of Venusian coronae, circular volcanic features unique to Venus. Coronae are thought to result from small instabilities (diapirs) from the core-mantle boundary, which are typical of stagnant-lid convection. However, most young coronae are located in a region surrounded by long-lived hotspots, typical of a more active style of mantle convection. Using analogue experiments in corn syrup heated from below, we show that the co-existence of diapirs and long-lived mantle plumes are a direct consequence of the catastrophic overturn of the cold Venusian lithosphere thought to have occurred ~ 700 Ma ago. In the last part we analyze the thermal effect of fluid flow through a full-scale experiment testing clay and concrete tunnel seals in a Deep Geological Repository for nuclear was finite element software, we were able to show that the formation of fissures in the heated chamber between the two seals effectively limited heat flow, and could explain the discrepancy between the predicted and measured temperatures.

Glass materials surround us, impacting our lives on a daily basis, whether geologically deposited by volcanic activity or synthesized in large volume by industry. These amorphous oxide materials are vastly important due to their variety of applications including solid electrolytes, cookware, and storage of high-level nuclear waste. Although they are used for different applications, one common characteristic of these materials is the absence of long-range periodic order. This makes it difficult to use traditional solid-state characterization methods such as x-ray and neutron diffraction to study glass structure. Nuclear magnetic resonance (NMR), is ideally suited to study materials that exhibit short-range non-periodic order as it probes directly at a nucleus of interest and is sensitive to its local structural environment. This ability of solid-state NMR is illustrated by revealing local structural features in various oxide materials presented in this thesis. Within is a compilation of studies looking at basic borates, followed by borovanadates and complex borosilicate glasses. A multinuclear application of using quantum chemical calculations, single and double resonance methods and charge-balance models are discussed to deconvolute the complex structures of these disordered materials. This is followed by a study of a difficult low-gamma nucleus, 73Ge, (once considered “impossible” for solid-state NMR) which is explored for future material studies by looking at 73Ge NMR of crystalline and glassy germanates. 73Ge chemical shifts were related to coordination environments and quadrupolar coupling constants were related to bond length distortions.

Glass materials surround us, impacting our lives on a daily basis, whether geologically deposited by volcanic activity or synthesized in large volume by industry. These amorphous oxide materials are vastly important due to their variety of applications including solid electrolytes, cookware, and storage of high-level nuclear waste. Although they are used for different applications, one common characteristic of these materials is the absence of long-range periodic order. This makes it difficult to use traditional solid-state characterization methods such as x-ray and neutron diffraction to study glass structure. Nuclear magnetic resonance (NMR), is ideally suited to study materials that exhibit short-range non-periodic order as it probes directly at a nucleus of interest and is sensitive to its local structural environment. This ability of solid-state NMR is illustrated by revealing local structural features in various oxide materials presented in this thesis. Within is a compilation of studies looking at basic borates, followed by borovanadates and complex borosilicate glasses. A multinuclear application of using quantum chemical calculations, single and double resonance methods and charge-balance models are discussed to deconvolute the complex structures of these disordered materials. This is followed by a study of a difficult low-gamma nucleus, 73Ge, (once considered “impossible” for solid-state NMR) which is explored for future material studies by looking at 73Ge NMR of crystalline and glassy germanates. 73Ge chemical shifts were related to coordination environments and quadrupolar coupling constants were related to bond length distortions.

The Institute of Resource Ecology (IRE) is one of the eight institutes of the Helmholtz-Zentrum Dresden – Rossendorf (HZDR). The research activities are mainly integrated into the program “Nuclear Waste Management, Safety and Radiation Research (NUSAFE)” of the Helmholtz Association (HGF) and focused on the topics “Safety of Nuclear Waste Disposal” and “Safety Research for Nuclear Reactors”. Additionally, various activities have been started investigating chemical and environmental aspects of processing and recycling of strategic metals, namely rare earth elements. These activities are located in the HGF program “Energy Efficiency, Materials and Resources (EMR)”. Both programs, and therefore all work which is done at IRE, belong to the research sector “Energy” of the HGF. The research objectives are the protection of humans and the environment from hazards caused by pollutants resulting from technical processes that produce energy and raw materials. Treating technology and ecology as a unity is the major scientific challenge in assuring the safety of technical processes and gaining their public acceptance. We investigate the ecological risks exerted by radioactive and nonradioactive metals in the context of nuclear waste disposal, the production of energy in nuclear power plants, and in processes along the value chain of metalliferous raw materials. A common goal is to generate better understanding about the dominating processes essential for metal mobilization and immobilization on the molecular level by using advanced spectroscopic methods. This in turn enables us to assess the macroscopic phenomena, including models, codes, and data for predictive calculations, which determine the transport and distribution of contaminants in the environment.

Flow instabilities occur at all scales in planetary systems. In this thesis we examine three cases of such instabilities, on three very different length scales. In the first part, we test the idea that Archean granite-greenstone belts (GGBs) form by crustal diapirism, or Rayleigh-Taylor instabilities. GGBs are characterized by large granitic domes (50-100 km in diameter) embedded in narrow keel-shaped greenstones. They are ubiquitous in Archean (> 2.5 Ga) terrains, but rare thereafter. We performed finite element calculations for a visco-elastic, temperature-dependent, non-Newtonian crust under conditions appropriate for the Archean, which show that dense low-viscosity volcanics overlying a felsic basement will overturn diapirically in as little as 10 Ma, displacing as much as 60 % of the volcanics to the lower crust. This surprisingly fast overturn rate suggests that diapiric overturn dominated crustal tectonics in the hot conditions of the Early Earth, becoming less important as the Earth cooled. Moreover, the deposition of large volumes of wet basaltic volcanics to the lower crust may provide the source for the formation of the distinctly Archean granitic rocks which dominate Earth's oldest continents. The second part examines the origin of Venusian coronae, circular volcanic features unique to Venus. Coronae are thought to result from small instabilities (diapirs) from the core-mantle boundary, which are typical of stagnant-lid convection. However, most young coronae are located in a region surrounded by long-lived hotspots, typical of a more active style of mantle convection. Using analogue experiments in corn syrup heated from below, we show that the co-existence of diapirs and long-lived mantle plumes are a direct consequence of the catastrophic overturn of the cold Venusian lithosphere thought to have occurred ~ 700 Ma ago. In the last part we analyze the thermal effect of fluid flow through a full-scale experiment testing clay and concrete tunnel seals in a Deep Geological Repository for nuclear was finite element software, we were able to show that the formation of fissures in the heated chamber between the two seals effectively limited heat flow, and could explain the discrepancy between the predicted and measured temperatures.