ALBERT

Description: Potash seams are a valuable resource containing several economically interesting, but also highly soluble minerals. In the presence of water, uncontrolled leaching can occur, endangering subsurface mining operations. In the present study, the influence of insoluble inclusions and intersecting layers on leaching zone evolution was examined by means of a reactive transport model. For that purpose, a scenario analysis was carried out, considering different rock distributions within a carnallite-bearing potash seam. The results show that reaction-dominated systems are not affected by heterogeneities at all, whereas transport-dominated systems exhibit a faster advance in homogeneous rock compositions. In return, the ratio of permeated rock in vertical direction is higher in heterogeneous systems. Literature data indicate that most natural potash systems are transport-dominated. Accordingly, insoluble inclusions and intersecting layers can usually be seen as beneficial with regard to reducing hazard potential as long as the mechanical stability of leaching zones is maintained. Thereby, the distribution of insoluble areas is of minor impact unless an inclined, intersecting layer occurs that accelerates leaching zone growth in one direction. Moreover, it is found that the saturation dependency of dissolution rates increases the growth rate in the long term, and therefore must be considered in risk assessments.

Description: Salt deposits offer a variety of usage types. These include the mining of rock salt and potash salt as important raw materials, the storage of energy in man-made underground caverns, and the disposal of hazardous substances in former mines. The most serious risk with any of these usage types comes from the contact with groundwater or surface water. It causes an uncontrolled dissolution of salt rock, which in the worst case can result in the flooding or collapse of underground facilities. Especially along potash seams, cavernous structures can spread quickly, because potash salts show a much higher solubility than rock salt. However, as their chemical behavior is quite complex, previous models do not account for these highly soluble interlayers. Therefore, the objective of the present thesis is to describe the evolution of cavernous structures along potash seams in space and time in order to improve hazard mitigation during the utilization of salt deposits. The formation of cavernous structures represents an interplay of chemical and hydraulic processes. Hence, the first step is to systematically investigate the dissolution and precipitation reactions that occur when water and potash salt come into contact. For this purpose, a geochemical reaction model is used. The results show that the minerals are only partially dissolved, resulting in a porous sponge like structure. With the saturation of the solution increasing, various secondary minerals are formed, whose number and type depend on the original rock composition. Field data confirm a correlation between the degree of saturation and the distance from the center of the cavern, where solution is entering. Subsequently, the reaction model is coupled with a flow and transport code and supplemented by a novel approach called ‘interchange’. The latter enables the exchange of solution and rock between areas of different porosity and mineralogy, and thus ultimately the growth of the cavernous structure. By means of several scenario analyses, cavern shape, growth rate and mineralogy are systematically investigated, taking also heterogeneous potash seams into account. The results show that basically four different cases can be distinguished, with mixed forms being a frequent occurrence in nature. The classification scheme is based on the dimensionless numbers Péclet and Damköhler, and allows for a first assessment of the hazard potential. In future, the model can be applied to any field case, using measurement data for calibration. The presented research work provides a reactive transport model that is able to spatially and temporally characterize the propagation of cavernous structures along potash seams for the first time. Furthermore, it allows to determine thickness and composition of transition zones between cavern center and unaffected salt rock. The latter is particularly important in potash mining, so that natural cavernous structures can be located at an early stage and the risk of mine flooding can thus be reduced. The models may also contribute to an improved hazard prevention in the construction of storage caverns and the disposal of hazardous waste in salt deposits. Predictions regarding the characteristics and evolution of cavernous structures enable a better assessment of potential hazards, such as integrity or stability loss, as well as of suitable mitigation measures.

Description: Salzlagerstätten bieten eine Vielzahl an Nutzungsmöglichkeiten. Diese umfassen den Abbau von Steinsalz und Kalisalz als wichtige Rohstoffe, die Speicherung von Energie in künstlich erzeugten Hohlräumen, sowie die Entsorgung gefährlicher Substanzen in stillgelegten Bergwerken. Die größte Gefahr bei jeder dieser Nutzungsarten ist der Kontakt mit Grund- oder Oberflächenwasser. Er bewirkt eine unkontrollierte Lösung des Salzgesteins, was im schlimmsten Fall zur Flutung oder zum Einsturz unterirdischer Infrastrukturen führt. Insbesondere entlang von Kaliflözen können sich kavernöse Strukturen schnell ausbreiten, da Kalisalze eine wesentlich höhere Löslichkeit besitzen als Steinsalz. Ihr chemisches Verhalten ist jedoch komplex, weshalb bisherige Modelle diese hochlöslichen Zwischenschichten vernachlässigen. Ziel der vorliegenden Doktorarbeit ist es daher, die Ausbreitung kavernöser Strukturen entlang von Kaliflözen räumlich und zeitlich zu beschreiben und damit die Möglichkeiten zur Gefahrenprävention bei der Nutzung von Salzlagerstätten zu verbessern. Die Bildung kavernöser Strukturen ist ein Zusammenspiel chemischer und hydraulischer Prozesse. Zunächst wird daher mithilfe eines geochemischen Reaktionsmodells systematisch untersucht, welche Lösungs- und Fällungsreaktionen beim Kontakt von Wasser und Kalisalz auftreten. Die Ergebnisse zeigen, dass nur ein Teil der Minerale gelöst wird, wodurch sich eine poröse, schwammartige Struktur bildet. Mit zunehmender Aufsättigung der Lösung treten verschiedene Sekundärminerale auf, deren Anzahl und Art vom Ausgangsgestein abhängen. Felddaten belegen dabei eine Korrelation zwischen Sättigungsgrad und Abstand vom Kavernenzentrum, wo die Lösung ein- und austritt. Anschließend wird das Reaktionsmodell mit einem Strömungs- und Transportcode gekoppelt und um einen neuartigen Ansatz namens "interchange" ergänzt. Dieser ermöglicht den Austausch von Lösung und Gestein zwischen Bereichen unterschiedlicher Porosität und Mineralogie, und damit letztlich das Wachstum der kavernösen Struktur. In mehreren Szenarienanalysen werden Kavernenform, Ausbreitungsgeschwindigkeit und Mineralogie systematisch untersucht und dabei auch heterogene Kaliflöze betrachtet. Die Ergebnisse zeigen, dass grundsätzlich vier Fälle zu unterscheiden sind, wobei in der Natur häufig Mischformen auftreten. Die Klassifizierung erfolgt auf Basis der dimensionslosen Kennzahlen Péclet und Damköhler und ermöglicht eine erste Abschätzung des Gefahrenpotentials. In Zukunft kann das Modell auf beliebige Feldbeispiele angewandt und mithilfe von Messdaten kalibriert werden. Die vorliegende Arbeit liefert ein reaktives Transportmodell, mit dem die Ausbreitung kavernöser Strukturen entlang von Kaliflözen erstmals räumlich und zeitlich beschrieben werden kann. Auch Mächtigkeit und Zusammensetzung der Übergangszone zwischen Kavernenzentrum und unberührtem Salzgestein können damit bestimmt werden. Letzteres ist insbesondere im Kalibergbau von Bedeutung, um natürliche kavernöse Strukturen rechtzeitig zu lokalisieren und damit das Risiko für eine Flutung von Bergwerken zu verringern. Auch bei der Herstellung von Speicherkavernen und der Einlagerung gefährlicher Substanzen im Salzgestein können die Modelle zu einer besseren Gefahrenprävention beitragen. Sie ermöglichen Prognosen über Beschaffenheit und Ausbreitungsverhalten kavernöser Strukturen, wodurch sowohl potentielle Gefahren, wie der Verlust von Dichtigkeit oder Stabilität, als auch geeignete Gegenmaßnahmen besser abschätzbar werden.

Description: Quantifying impacts on the environment and human health is a critical requirement for geological subsurface utilisation projects. In practice, an easily accessible interface for operators and regulators is needed so that risks can be monitored, managed, and mitigated. The primary goal of this work was to create an environmental hazards quantification toolkit as part of a risk assessment for in-situ coal conversion at two European study areas: the Kardia lignite mine in Greece and the Máza-Váralja hard coal deposit in Hungary, with complex geological settings. A substantial rock volume is extracted during this operation, and a contaminant pool is potentially left behind, which may put the freshwater aquifers and existing infrastructure at the surface at risk. The data-driven, predictive tool is outlined exemplary in this paper for the Kardia contaminant transport model. Three input parameters were varied in a previous scenario analysis: the hydraulic conductivity, as well as the solute dispersivity and retardation coefficient. Numerical models are computationally intensive, so the number of simulations that can be performed for scenario analyses is limited. The presented approach overcomes these limitations by instead using surrogate models to determine the probability and severity of each hazard. Different surrogates based on look-up tables or machine learning algorithms were tested for their simplicity, goodness of fit, and efficiency. The best performing surrogate was then used to develop an interactive dashboard for visualising the hazard probability distributions. The machine learning surrogates performed best on the data with coefficients of determination R2〉0.98, and were able to make the predictions quasi-instantaneously. The retardation coefficient was identified as the most influential parameter, which was also visualised using the toolkit dashboard. It showed that the median values for the contaminant concentrations in the nearby aquifer varied by five orders of magnitude depending on whether the lower or upper retardation range was chosen. The flexibility of this approach to update parameter uncertainties as needed can significantly increase the quality of predictions and the value of risk assessments. In principle, this newly developed tool can be used as a basis for similar hazard quantification activities.

Description: In the context of a potential utilisation of coal resources located in the Mecsek mountain area in Southern Hungary, an assessment of groundwater pollution resulting from a potential water-borne contaminant pool remaining in in situ coal conversion reactors after site abandonment has been undertaken in the scope of the present study. The respective contaminants may be of organic and inorganic nature. A sensitivity analysis was carried out by means of numerical simulations of fluid flow as well as contaminant and heat transport including retardation to assess spatial contaminant migration. Hereby, the main uncertainties, e.g., changes in hydraulic gradient and hydraulic contributions of the complex regional and local fault systems in the study area, were assessed in a deterministic way to identify the relevant parameters. Overall 512 simulations of potential groundwater contamination scenarios within a time horizon exceeding the local post-operational monitoring period were performed, based on maximum contaminant concentrations, cumulative mass balances as well as migration distances of the contaminant plume. The simulation results show that regional faults represent the main contaminant migration pathway, and that contamination is unlikely assuming the given reference model parametrisation. However, contamination within a simulation time of 50 years is possible for specific geological conditions, e.g., if the hydraulic conductivity of the regional faults exceeds a maximum value of 1 × 10−5 m s−1. Further, the parameter data analysis shows that freshwater aquifer contamination is highly non-linear and has a bimodal distribution. The bivariate correlation coefficient heatmap shows slightly positive correlations for the pressure difference, the fault permeability and the simulation time, as well as a negative correlation for the retardation coefficient. The results of this sensitivity analysis have been integrated into a specific toolkit for risk assessment for that purpose.

Description: Many types of geologic subsurface utilisation are associated with fluid and heat flow as well as simultaneously occurring chemical reactions. For that reason, reactive transport models are required to understand and reproduce the governing processes. In this regard, reactive transport codes must be highly flexible to cover a wide range of applications, while being applicable by users without extensive programming skills at the same time. In this context, we present an extension of the Open Source and Open Access TRANSPORT Simulation Environment, which has been coupled with the geochemical reaction module PHREEQC, and thus provides multiple new features that make it applicable to complex reactive transport problems in various geoscientific fields. Code readability is ensured by the applied high-level programming language Python which is relatively easy to learn compared to low-level programming languages such as C, C++ and FORTRAN. Thus, also users with limited software development knowledge can benefit from the presented simulation environment due to the low entry-level programming skill requirements. In the present study, common geochemical benchmarks are used to verify the numerical code implementation. Currently, the coupled simulator can be used to investigate 3D single-phase fluid and heat flow as well as multicomponent solute transport in porous media. In addition to that, a wide range of equilibrium and nonequilibrium reactions can be considered. Chemical feedback on fluid flow is provided by adapting porosity and permeability of the porous media as well as fluid properties. Thereby, users are in full control of the underlying functions in terms of fluid and rock equations of state, coupled geochemical modules used for reactive transport, dynamic boundary conditions and mass balance calculations. Both, the solution of the system of partial differential equations and the PHREEQC module, can be easily parallelised to increase computational efficiency. The benchmarks used in the present study include density-driven flow as well as advective, diffusive and dispersive reactive transport of solutes. Furthermore, porosity and permeability changes caused by kinetically controlled dissolution-precipitation reactions are considered to verify the main features of our reactive transport code. In future, the code implementation can be used to quantify processes encountered in different types of subsurface utilisation, such as water resource management as well as geothermal energy production, as well as geological energy, CO2 and nuclear waste storage.

Description: Im Rahmen der derzeit stattfindenden Variantenuntersuchung zur Erneuerung der Fehmarnsundquerung wurde in verschiedenen Tiefen Tarraston angetroffen. Wie schon bei den Baumaßnahmen vor 50 Jahren stellt dieser eine ernste Herausforderung dar. Insbesondere das Quell‐ und Schwellverhalten des Tons sowie seine geringe Scherfestigkeit im Bereich von Harnischflächen könnten beim Bau der neuen Brücke bzw. des Tunnels Probleme bereiten. Dieser Artikel vergleicht verschiedene als Tarraston eingestufte Proben im Hinblick auf ihre Zusammensetzung, ihre Mikrostruktur und ihr Quellverhalten und zeigt dabei Zusammenhänge auf. So konnte gezeigt werden, dass die Kornverteilung der untersuchten Proben des Tarrastons keine sichere Aussage über deren Quellverhalten zulässt, während Plastizität oder Wasseraufnahmevermögen zuverlässige Anhaltspunkte bieten. Zwei Tone, die sich in granulometrischer und tonmineralogischer Zusammensetzung sowie Setzungsverhalten kaum unterscheiden, wiesen beim Quellverhalten deutliche Unterschiede auf. Der Artikel diskutiert die Ursachen und geht dabei auch auf die Mikrostruktur des Tarrastons ein. Ferner werden die Versuchsergebnisse mit Literaturwerten des besser erforschten London Clay verglichen.

Description: Brine occurrences belong to the most significant risks in salt mining as they can lead to mine flooding and land subsidence. Especially within highly soluble potash seams, which contain some of the economically most interesting types of salt, the interactions between brine and salt rock result in cavernous structures surrounded by moisture penetration zones with different mineralogical regions. In order to facilitate an early detection of cavernous structures, the brine and rock composition along these transition zones was modelled. The results show that the potash salt composition, or more precisely the ratio between kieserite and sylvite, determines the dissolution behaviour and, therefore, which types of secondary minerals occur. According to the volume balance, cavitation is only possible close to the centre of a cavernous structure, where the solid-fluid-ratio is low. Furthermore, an open system with frequent brine exchange is required. Along the transition zone, the solid-fluid-ratio can increase to several tens of kilograms before the water is fully consumed and the unaffected salt rock is reached. A comparison with measured data from a natural brine occurrence validates the model results and confirms a correlation between the brine composition and the distance from the centre of a cavernous structure. In conclusion, the models are suitable to determine the location of the central part of a cavernous structure based on rock and brine samples from the vicinity. However, in order to simulate the temporal and spatial development of geogenic cavities, a coupling of chemistry and hydraulics will be necessary.

Description: Potash salts belong to the most soluble minerals and their unintended dissolution can result in a safety risk for the construction and utilisation of salt caverns and mines [1]. One main challenge in modelling the formation of leaching zones within potash seams is the representation of fluid-rock interactions within regions exhibiting highly varying porosities. Chemical reactions cannot take place if small porosities inhibit the inflow of solution, although present solutions may be undersaturated with respect to certain minerals. These porosity variations only occur at the dissolution front in binary systems, such as NaCl solution and solid halite. Its progress can be described by a mass transfer rate, depending on the concentration of present solutions or by assuming a saturated interface between dry rock and solution, subtracting out the diffusive mass transport. In contrast, the dissolution of potash salt results in the formation of a porous rock matrix, consisting of undissolved and precipitated minerals that can further react with the surrounding solution. Accordingly, fluid-rock interactions and largely varying porosities also occur remote from the dissolution front. The interchange approach [2] was developed to describe these interactions. Coupled with a reactive transport model including PHREEQC [3] and TRANSE [4] this approach is capable to quantify, e.g., the leaching process of carnallite-bearing potash seams due to natural density-driven convection. The dissolution rate is essential for both, the timely progress and geometric shape of evolving leaching zones in the potash seam. Therefore, the interchange approach has been adapted in the scope of the present study to consider saturation-dependent dissolution rates for each mineral. In this contribution, we discuss the feasibility and limitations of our approach to represent fluid-rock interactions between brine and different types of potash salts at the metre scale.

Description: Leaching zones within potash seams generally represent a significant risk to subsurface mining operations and the construction of technical caverns in salt rocks, but their temporal and spatial formation has been investigated only rudimentarily to date. To the knowledge of the authors, current reactive transport simulation implementations are not capable to address hydraulic-chemical interactions within potash salt. For this reason, a reactive transport model has been developed and complemented by an innovative approach to calculate the interchange of minerals and solution at the water-rock interface. Using this model, a scenario analysis was carried out based on a carnallite-bearing potash seam. The results show that the evolution of leaching zones depends on the mineral composition and dissolution rate of the original salt rock, and that the formation can be classified by the dimensionless parameters of Péclet (Pe) and Damköhler (Da). For Pe 〉 2 and Da 〉 1, a funnel-shaped leaching zone is formed, otherwise the dissolution front is planar. Additionally, Da 〉 1 results in the formation of a sylvinitic zone and a flow barrier. Most scenarios represent hybrid forms of these cases. The simulated shapes and mineralogies are confirmed by literature data and can be used to assess the hazard potential.

Description: Multicomponent DNAPL pools are among the most common reasons for groundwater contamination and represent highly persistent source areas. Although several studies have already shown that their constituents influence each other’s solubility, existing models neglect these interactions. For this reason, a semi-analytical model has been developed, considering the pool composition as temporally variable. Based on Raoult’s law, the molar fraction, the effective solubility and finally the mass discharge due to advection, dispersion and diffusion of each component are determined. The results significantly differ from studies on single-phase pools. It is shown that mass discharges can both increase and decrease over time and that the longevity of DNAPL pools as well as the time until threshold values are fullfilled will be significantly underestimated if Raoult’s law is neglected. Additionally, a sensitivity analysis reveals that poorly soluble minor components must not be neglected, whereas highly soluble ones can.