Dynamic Evolution of Permeability in Response to Chemo‐Mechanical Compaction

Pressure‐solution creep is an important fluid‐mediated deformation mechanism, causing chemo‐mechanical transformations and porosity and permeability changes in rocks. The presence of phyllosilicates, in particular, has previously been hypothesized to further reduce porosity and pore connectivity. Nevertheless, a full characterization of the spatio‐temporal evolution of permeability during this process has yet to be reported. A pure NaCl aggregate and a mixture of NaCl and biotite were deformed through pressure‐solution creep while monitoring their microstructural evolution through computed X‐ray micro‐tomography. The evolution of permeability and fluid velocity of the samples were computed by using the pore geometries from the X‐ray micro‐tomography as input for the Lattice‐Boltzmann modeling. The results indicate that, as deformation proceeds, porosity and permeability decrease in both samples. In the salt ‐biotite sample pressure solution creep causes the formation of a compaction band perpendicular to the direction of loading, forming a barrier for permeability. Along the other two directions, pore connectivity and permeability are retained in the marginal salt layers, making the sample strongly anisotropic. The presence of biotite controls the way pore coordination number evolves and hence, the connectivity of the pathways. Biotite flakes create an enhanced porosity decrease leading to compaction and reduction of pore connectivity. This reduction in porosity affects local stresses and local contact areas, reducing over time the driving force. According to a texture‐porosity process, the reduction in porosity causes salt ions to dissolve in the marginal salt and precipitate within the biotite‐bearing layer, where the bulk volume of salt grains increases over time

4D porosity evolution during pressure-solution of NaCl in the presence of phyllosilicates

Pressure-solution creep is one of the most common crustal deformation mechanisms, inducing changes in the porosity and permeability of rocks. For a variety of rock types undergoing pressure solution, it has been shown that the presence of phyllosilicates may significantly enhance the rate of the pressure-solution process. In this experimental investigation, we present 4-dimensional (three dimensions + time) X-ray microtomographic data that contrast deformation by pressure-solution of a pure NaCl aggregate with that of a mixture of NaCl and biotite. The results show that for mixed samples (NaCl+biotite), phyllosilicates induce a marked reduction in porosity and pore connectivity and contribute to an increase in the local strain rates by an order of magnitude over pure NaCl samples. At the same time, phyllosilicates do not induce strain localization in the sample. We discuss various possible explanations for these observations including a possible positive feedback between the porosity distribution and pressure solution. Our study yields novel insights into the local effects of phyllosilicates during pressure-solution creep and provides full 4-dimensional imaging and characterization of the coupled evolution of porosity and pore connectivity over previously unprecedented experimental time scales

Microstructural analysis of slag properties associated with calcite precipitation due to passive CO2 mineralization

CO2 mineralization in slag has gained significant attention since it occurs with minimal human intervention and energy input. While the amount of theoretical CO2 that can be captured within slag has been quantified based on slag composition in several studies, the microstructural and mineralogical effects of slag on its ability to capture CO2 have not been fully addressed. In this work, the CO2 uptake within legacy slag samples is analyzed through microstructural characterization. Slag samples were collected from the former Ravenscraig steelmaking site in Lanarkshire, Scotland. The collected samples were studied using X-ray Computed Tomography (XCT) to understand the distribution and geometry of pore space, as well as with scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectroscopy (EDS) to visualize the distribution of elements within the studied samples. Electron backscatter diffraction (EBSD) was used to study the minerals distribution. The samples were also characterized through X-ray diffraction (XRD) and X-ray fluorescence (XRF), and the amount of captured CO2 was quantified using thermogravimetric analysis (TGA). Our results demonstrate that CO2 uptake occurs to the extent of ∼9–30g CO2/ kg slag. The studied samples are porous in nature, with pore space occupying up to ∼30% of their volumes, and they are dominated by åkermanite-gehlenite minerals which interact with the atmospheric CO2 slowly at ambient conditions. EDS and EBSD results illustrate that the precipitated carbonate in slag is calcite, and that the precipitation of calcite is accompanied by the formation of a Si-O-rich layer. The provided analysis concludes that the porous microstructure as well as the minerals distribution in slag should be considered in forecasting and designing large-scale solutions for passive CO2 mineralization in slag

A separated vortex ring underlies the flight of the dandelion

Wind-dispersed plants have evolved ingenious ways to lift their seeds1,2. The common dandelion uses a bundle of drag-enhancing bristles (the pappus) that helps to keep their seeds aloft. This passive flight mechanism is highly effective, enabling seed dispersal over formidable distances3,4; however, the physics underpinning pappus-mediated flight remains unresolved. Here we visualized the flow around dandelion seeds, uncovering an extraordinary type of vortex. This vortex is a ring of recirculating fluid, which is detached owing to the flow passing through the pappus. We hypothesized that the circular disk-like geometry and the porosity of the pappus are the key design features that enable the formation of the separated vortex ring. The porosity gradient was surveyed using microfabricated disks, and a disk with a similar porosity was found to be able to recapitulate the flow behaviour of the pappus. The porosity of the dandelion pappus appears to be tuned precisely to stabilize the vortex, while maximizing aerodynamic loading and minimizing material requirements. The discovery of the separated vortex ring provides evidence of the existence of a new class of fluid behaviour around fluid-immersed bodies that may underlie locomotion, weight reduction and particle retention in biological and manmade structures

Brecciation at the grain scale within the lithologies of the Winchcombe Mighei‐like carbonaceous chondrite

The Mighei‐like carbonaceous (CM) chondrites have been altered to various extents by water–rock reactions on their parent asteroid(s). This aqueous processing has destroyed much of the primary mineralogy of these meteorites, and the degree of alteration is highly heterogeneous at both the macroscale and nanoscale. Many CM meteorites are also heavily brecciated juxtaposing clasts with different alteration histories. Here we present results from the fine‐grained team consortium study of the Winchcombe meteorite, a recent CM chondrite fall that is a breccia and contains eight discrete lithologies that span a range of petrologic subtypes (CM2.0–2.6) that are suspended in a cataclastic matrix. Coordinated multitechnique, multiscale analyses of this breccia reveal substantial heterogeneity in the extent of alteration, even in highly aqueously processed lithologies. Some lithologies exhibit the full range and can comprise nearly unaltered coarse‐grained primary components that are found directly alongside other coarse‐grained components that have experienced complete pseudomorphic replacement by secondary minerals. The preservation of the complete alteration sequence and pseudomorph textures showing tochilinite–cronstedtite intergrowths are replacing carbonates suggest that CMs may be initially more carbonate rich than previously thought. This heterogeneity in aqueous alteration extent is likely due to a combination of microscale variability in permeability and water/rock ratio generating local microenvironments as has been established previously. Nevertheless, some of the disequilibrium mineral assemblages observed, such as hydrous minerals juxtaposed with surviving phases that are typically more fluid susceptible, can only be reconciled by multiple generations of alteration, disruption, and reaccretion of the CM parent body at the grain scale

Brecciation at the grain scale within the lithologies of the Winchcombe Mighei-like carbonaceous chondrite

The Mighei‐like carbonaceous (CM) chondrites have been altered to various extents by water–rock reactions on their parent asteroid(s). This aqueous processing has destroyed much of the primary mineralogy of these meteorites, and the degree of alteration is highly heterogeneous at both the macroscale and nanoscale. Many CM meteorites are also heavily brecciated juxtaposing clasts with different alteration histories. Here we present results from the fine‐grained team consortium study of the Winchcombe meteorite, a recent CM chondrite fall that is a breccia and contains eight discrete lithologies that span a range of petrologic subtypes (CM2.0–2.6) that are suspended in a cataclastic matrix. Coordinated multitechnique, multiscale analyses of this breccia reveal substantial heterogeneity in the extent of alteration, even in highly aqueously processed lithologies. Some lithologies exhibit the full range and can comprise nearly unaltered coarse‐grained primary components that are found directly alongside other coarse‐grained components that have experienced complete pseudomorphic replacement by secondary minerals. The preservation of the complete alteration sequence and pseudomorph textures showing tochilinite–cronstedtite intergrowths are replacing carbonates suggest that CMs may be initially more carbonate rich than previously thought. This heterogeneity in aqueous alteration extent is likely due to a combination of microscale variability in permeability and water/rock ratio generating local microenvironments as has been established previously. Nevertheless, some of the disequilibrium mineral assemblages observed, such as hydrous minerals juxtaposed with surviving phases that are typically more fluid susceptible, can only be reconciled by multiple generations of alteration, disruption, and reaccretion of the CM parent body at the grain scale

Four-dimensional studies of fluid-rock interaction

Successful management of hydrocarbon reservoirs, geothermal energy extraction sites, radioactive waste and CO2 storage sites depends on a detailed knowledge of fluid transport properties, porosity and permeability. Amongst deformation processes, fluid-rock interaction plays an important role in controlling the petrophysical properties of a rock. The presence of fluids in the rocks induce chemical and physical changes in compositions and texture, affecting porosity and permeability, hence influencing dynamic transport properties and fluid flow. Fluid-rock interaction processes have been deeply investigated in nature and in numerous experimental and numerical modelling studies. However, these studies lack a spatio-temporal characterization of the dynamic evolution of porosity and reaction microfabrics. There is no clear understanding of the spatio-temporal evolution of these properties in three dimensions, and how this evolution affects fluid percolation in the rock. Computed X-ray micro-Tomography (μCT) was applied to investigate these processes in three dimensions and observe their evolution in time (4DμCT). The combination of μCT with 2D analytical techniques (e.g. scanning electron microscope, SEM, electron microcrobe, EMPA, electron backscatter diffraction, EBSD) furthermore enables the extrapolation of the information gained from 2D analyses to the 3rd an 4th dimension (4D μCT). The thesis investigates two different categories of fluid-rock interaction processes, by using 4DμCT to monitor the evolution of mineral reactions (in the first case) and porosity (second case) in relation to strain and time. In the first case study, natural rock samples were analysed. The samples show a compositional change along a strain gradient from olivinic metagabbros to omphacite-garnet bearing eclogites in a ductile shear zone. Synchroton-based x-ray microtomography (sμCT) was applied to document the 3D evolution of garnets along the strain gradient (which represent the 4th dimension). The 3D spatial arrangement of garnet microfabrics can help determine the deformation history and the extent of fluid-rock interaction active during deformation. Results from the sμCT show that in the low strain domain, garnets form a large and well interconnected cluster that develops throughout the entire sample and garnet coronas never completely encapsulate olivine grains. In the most highly deformed eclogites, the oblate shapes of garnets reflect a deformational origin of the microfabrics. EBSD analyses reveal that garnets do not show evidence for crystal plasticity, but rather they highlight evidence for minor fracturing, neo-nucleation and overgrowth, which points to a mechanical disintegration of the garnet coronas during strain localisation. In the second case study, pressure-solution processes were investigated using NaCl as rock-analogue, to monitor the evolution of porosity and pore connectivity in four dimensions, providing a time-resolved characterization of the processes. NaCl samples were uniaxially compacted and μCT scans were taken at regular interval times to characterize the evolution of grain morphologies, pore space and macro-connectivity of the samples. Different uniaxial loads, as well as different bulk sample compositions (phyllosilicates and/or glass beads) were used to investigate their effect on the process. Greater uniaxial loads, and the presence of phyllosilicates within the deforming NaCl columns were found to enhance pressure-solution processes. The pore space becomes highly disconnected in the presence of phyllosilicates, with important implications for fluid percolation and dynamic transport properties. Mean strain rates, calculated from volumetric Digital Image Correlation (3D-DIC) analyses, were found to be higher where phyllosilicates were located. The combination of μCT with volumetric DIC and SEM imaging proved to be an efficient analytical method for investigating the dynamic behaviour of porosity and permeability during ongoing pressure-solution processes. The results showed that fluid-rock interaction critically modifies the rocks at the pore/grain scale, with important consequences on dynamic fluid transport properties. The combination of μCT with classical 2D techniques provided a better understanding on the dynamic evolution of transport properties and fluid percolation during fluid-rock interaction processes, allowing the characterization in three dimensions of reaction microfabrics and porosity

Analisi strutturale della deformazione alpina nei granitoidi dei Tauri nell'area delle Mesule (Alto Adige-Südtirol, Italia): interazione fra deformazione fragile e duttile durante condizioni metamorfiche in facies anfibolitica

The aim of the present work is the study of the Alpine deformation in the area of the Mesuler glacier, near the Neves Lake, in Alto Adige –Südtirol (Italy). In the Neves area the deformation is localized within metagranitoids belonging to the Zentralgneiss Penninic unit of the Tauern Window; the pre-Alpine granitoids were deformed during the Alpine orogeny under amphibolites facies metamorphic conditions, and were converted to orthogneiss and mylonites. Specific objectives of the thesis are: i) the study of the interaction between ductile and brittle deformation during the high-grade metamorphic conditions, with a particular focus on the development of quartz veins during a prevailing ductile deformation; ii) the organization of a database and analysis in a GIS environment of the bulk structural data collected in numerous previous investigations of the area. With regard to the quartz veins, it was performed an analysis of different types of geometries and their kinematic relationships associated with ductile structures. Unfortunately a preliminary attempt at reconstructing 3D geometry of the veins by Ground Penetrating Radar (GPR) failed. We also analyzed the field geometry of veins in terms of the kinematics of vein opening and cycles of fluid pressure during ongoing deformation. The fluid-rock interaction during vein formation was investigated by the analysis of thin sections of the alteration haloes surrounding the veins and by geochemical analysis of the altered zones. Some quartz veins were used for the study of fluid inclusions to constrain the conditions of formation

The Utilisation of X-ray Micro-Computed Tomography (XCT) for the Quantification of Carbon Dioxide in Passively Carbonated Steel Slag

Mineral sequestration using solid alkaline by-products, such as steel slag, is a feasible technology to capture carbon dioxide. This silicate weathering reaction forms solid carbonates, mineralizing the atmospheric CO2 into calcite, which can occur passively under ambient environmental conditions over monthly to decadal timescales. The passive mineralization of carbon dioxide in steel slag is a not well-known reaction, particularly when climate factors influence the mineral carbonation. Non-destructive quantification of CO2 mineralization is necessary to set underpinning knowledge on capturing rates. The utilisation of X-ray micro-Computed Tomography (XCT) allows the 3D spatial visualisation and quantification of carbon dioxide precipitated as calcite in steel slag pores. We used XCT to analyse samples of legacy steel slag collected in Mexico and Scotland, to determine the effects of environmental factors on mineral carbonation. The XCT data were analysed with image processing to classify the slag volume into three phases (slag, pores, and calcite). The classification of the data into different phases allows the determination of the volume of each phase in the sample as well as its 3D spatial extent, thus enabling the quantification of mineralized CO2 characterized as the calcite phase. We will present a comparison between the volumes of carbon dioxide passively mineralized in the samples from the Mexican and Scottish collection sites, in the context of contrasting environmental factors. Preliminary results from one of the Scottish samples shows that calcite (mineralized CO2) accounts for ~ 5 vol. % of the sample, and it is localised across the whole sample. A comparison of these results between the Mexican and Scottish samples will provide a better understanding of how climatic factors influence the volumes of atmospheric CO2 mineralized by the samples