ALBERT

Description: Establishing models for the formation of well-mixed polyphase domains in ultramylonites is difficult because the effects of large strains and thermo-hydro-chemo-mechanical feedbacks can obscure the transient phenomena that may be responsible for domain production. We use scanning electron microscopy and nanotomography to offer critical insights into how the microstructure of a highly deformed quartzo-feldspathic ultramylonite evolved. The dispersal of monomineralic quartz domains in the ultramylonite is interpreted to be the result of the emergence of synkinematic pores, called creep cavities. The cavities can be considered the product of two distinct mechanisms that formed hierarchically: Zener–Stroh cracking and viscous grain-boundary sliding. In initially thick and coherent quartz ribbons deforming by grain-size-insensitive creep, cavities were generated by the Zener–Stroh mechanism on grain boundaries aligned with the YZ plane of finite strain. The opening of creep cavities promoted the ingress of fluids to sites of low stress. The local addition of a fluid lowered the adhesion and cohesion of grain boundaries and promoted viscous grain-boundary sliding. With the increased contribution of viscous grain-boundary sliding, a second population of cavities formed to accommodate strain incompatibilities. Ultimately, the emergence of creep cavities is interpreted to be responsible for the transition of quartz domains from a grain-size-insensitive to a grain-size-sensitive rheology.

Description: The olivine carbonation reaction, in which carbon dioxide is chemically incorporated to form carbonate, is central to the emerging carbon sequestration method using ultramafic rocks. The rate of this retrograde metamorphic reaction is controlled, in part, by the available reactive surface area: as the solid volume increases during carbonation, the feasibility of this method ultimately depends on the maintenance of porosity and the creation of new reactive surfaces. We conducted in situ dynamic X-ray microtomography and nanotomography experiments to image and quantify the porosity generation during olivine carbonation. We designed a sample setup that included a thick-walled cup (made of porous olivine aggregates with a mean grain size of either  ∼  5 or  ∼  80 µm) filled with loose olivine sands with grain sizes of 100–500 µm. The whole sample assembly was reacted with a NaHCO3 aqueous solution at 200 °C, under a constant confining pressure of 13 MPa and a pore pressure of 10 MPa. Using synchrotron-based X-ray microtomography, the three-dimensional (3-D) pore structure evolution of the carbonating olivine cup was documented until the olivine aggregates became disintegrated. The dynamic microtomography data show a volume reduction in olivine at the beginning of the reaction, indicating a vigorous dissolution process consistent with the disequilibrium reaction kinetics. In the olivine cup with a grain size of  ∼  80 µm (coarse-grained cup), dissolution planes developed within 30 h, before any precipitation was observed. In the experiment with the olivine cup of  ∼  5 µm mean grain size (fine-grained cup), idiomorphic magnesite crystals were observed on the surface of the olivine sands. The magnesite shows a near-constant growth throughout the experiment, suggesting that the reaction is self-sustained. Large fractures were generated as the reaction proceeded and eventually disintegrated the aggregate after 140 h. Detailed analysis show that these are expansion cracks caused by the volume mismatch in the cup walls, between the expanding interior and the near-surface which keeps a nearly constant volume. Nanotomography images of the reacted olivine cup reveal pervasive etch pits and wormholes in the olivine grains. We interpret this perforation of the solids to provide continuous fluid access, which is likely key to the complete carbonation observed in nature. Reactions proceeding through the formation of nano- to micron-scale dissolution channels provide a viable microscale mechanism in carbon sequestration practices. For the natural peridotite carbonation, a coupled mechanism of dissolution and reaction-induced fracturing should account for the observed self-sustainability of the reaction.

Description: The dispersal of monomineralic quartz domains in a quartzofeldspathic ultramylonite is interpreted to be the result of the emergence of syn-kinematic pores, called creep cavities. The cavities can be considered the product of two distinct mechanisms that formed hierarchically: Zener-Stroh cracking and viscous grain boundary sliding. In initially thick and coherent quartz ribbons deforming by grain size-insensitive creep, cavities were generated by the Zener-Stroh mechanism on grain-boundaries aligned with the YZ plane of finite strain. The opening of creep cavities promoted the ingress of fluids to sites of low stress. The local addition of a fluid lowered the adhesion and cohesion of grain-boundaries and promoted viscous grain boundary sliding. With the increased contribution of viscous grain boundary sliding, a second population of cavities formed to accommodate strain incompatibilities. Ultimately, the emergence of creep cavities is interpreted to be responsible for the transition of quartz domains from a grain size-insensitive, to a grain size-sensitive rheology.

Description: The olivine carbonation reaction, in which carbon dioxide is chemically incorporated to form carbonate, is central to the emerging carbon sequestration method using ultramafic rocks. The rate of this retrograde metamorphic reaction is controlled, in part, by the available reactive surface area: as the solid volume increases during carbonation, the feasibility of this method ultimately depends on the maintenance of porosity and the creation of new reactive surfaces. We conducted in-situ dynamic x-ray microtomography and nanotomography experiments to image and quantify the porosity generation during olivine carbonation. We designed a sample setup that included a thick-walled cup (made of porous olivine aggregates with a mean grain size of either ~ 5 or ~ 80 μm) filled with loose olivine sands with grain sizes of 100–500 μm. The whole sample assembly was reacted with a NaHCO3 aqueous solution at 200 °C, under a constant confining pressure of 13 MPa and a pore pressure of 10 MPa. Using synchrotron-based X-ray microtomography, the 3-dimensional (3-D) pore structure evolution of the carbonating olivine cup was documented until the olivine aggregates became disintegrated. The dynamic microtomography data show a volume reduction in olivine at the beginning of the reaction, indicating a vigorous dissolution process consistent with the disequilibrium reaction kinetics. In the olivine cup with a grain size of ~ 80 μm (coarse-grained cup), dissolution fractures developed within 30 hours, before any precipitation was observed. In the experiment with the olivine cup of ~ 5 μm mean grain size (fine-grained cup), idiomorphic magnesite crystals were observed on the surface of the olivine sands. The magnesite shows a near constant growth throughout the experiment, suggesting that the reaction is self-sustained. Large fractures were generated as reaction proceeds and eventually disintegrate the aggregate after 140 hours. Detailed analysis show that these are expansion cracks caused by the volume mismatch between the expanding interior and the nearly constant surface. Nanotomography images of the reacted olivine cup reveal pervasive etch-pits and worm-holes in the olivine grains. We interpret this perforation of the solids to provide continuous fluid access, which is likely key to the complete carbonation observed in nature. Reactions proceeding through the formation of nano- to micron-scale dissolution channels provide a viable microscale mechanism in carbon sequestration practices. For the natural peridotite carbonation, a coupled-mechanism of dissolution and reaction-induced fracturing should account for the observed self sustainability of the reaction.

Description: In experiments designed to understand deep shear zones, we show that periodic porous sheets emerge spontaneously during viscous creep and that they facilitate mass transfer. These findings challenge conventional expectations of how viscosity in solid rocks operates and provide quantitative data in favour of an alternative paradigm, that of the dynamic granular fluid pump model. On this basis, we argue that our results warrant a reappraisal of the community's perception of how viscous deformation in rocks proceeds with time and suggest that the general model for deep shear zones should be updated to include creep cavitation. Through our discussion we highlight how the integration of creep cavitation, and its Generalised Thermodynamic paradigm, would be consequential for a range of important solid Earth topics that involve viscosity in Earth materials like, for example, slow earthquakes.