Mineral carbonation, a process that binds CO2 in the form of carbonates by silicate weathering, is widespread on the Earth's surface. Because of the abundance of silicate rocks and the permanence of the carbonated solids, sequestering CO2 via mineral carbonation has generated lots of interests. However, it is unclear how the fluid‐rock reaction proceeds to completion in spite of an increasing solid volume. We conducted a mineral carbonation experiment in which a sintered olivine aggregate reacted with a sodium bicarbonate solution at reservoir conditions. Time‐resolved synchrotron X‐ray microtomographic images show cracks in polygonal patterns arising in the surface layers and propagating into the interior of the olivine aggregate. The nanotomography data reveal that the incipient cracks intersect at right angles. We infer that stretching due to nonuniform volume expansion generates polygonal cracking of the surfaces. Our data shed new lights on the processes that control hydration and carbonation of peridotite.

We conducted experiments to investigate the influence of pore fluid pressure on the frictional strength and slip behavior of gouge bearing faults. Saw cut porous sandstone samples with a layer of gouge powders placed between the precut surfaces were deformed in the conventional triaxial loading configuration. A series of velocity‐step tests were performed to measure the response of the friction coefficient to variations in sliding velocity. Pore volume changes were monitored during shearing of the gouge. Our results demonstrate that under constant effective pressure, increasing pore pressure stabilizes the frictional slip of faults with all four gouge materials including antigorite, olivine, quartz, and chrysotile. The stabilizing effect is the strongest in antigorite gouge, which shows an evolution of friction parameters from velocity‐weakening toward velocity‐strengthening behavior with increasing pore pressure. Experiments with controlled pore volume show that the pore volume reduction diminishes under high pore fluid pressures, implying an increasing dilation component at these conditions. The dilatant hardening mechanism can explain the observed strengthening. These results provide a possible explanation to the observed spatial correlation between slow slip events and high pore pressure in many subduction zones.

Abstract. 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.

Olivine and pyroxene‐bearing rocks in the oceanic crust react with hydrothermal fluids producing changes in the physical characteristics and behaviors of the altered rocks. Notably, these reactions tend to increase solid volume, reducing pore volume, permeability, and available reactive surface area, yet entirely hydrated and/or carbonated rocks are commonly observed in the field. We investigate the evolution of porosity and permeability of fractured dunites reacted with CO2‐rich solutions in laboratory experiments. The alteration of crack surfaces changes the mechanical and transport properties of the bulk samples. Analysis of three‐dimensional microstructural data shows that although precipitation of secondary minerals causes the total porosity of the sample to decrease, an interconnected network of porosity is maintained through channelized dissolution and coupled carbonate precipitation. The observed microstructure appears to be the result of chemo‐mechanical coupling, which may provide a mechanism of porosity maintenance without the need to invoke reaction‐driven cracking.

Abstract. Geological carbon sequestration provides permanent CO2 storage to mitigate the current high concentration of CO2 in the atmosphere. CO2 mineralization in basalts has been proven to be one of the most secure storage options. For successful implementation and future improvements of this technology, the time-dependent deformation behavior of reservoir rocks in the presence of reactive fluids needs to be studied in detail. We conducted load-stepping creep experiments on basalts from the CarbFix site (Iceland) under several pore fluid conditions (dry, H2O saturated and H2O + CO2 saturated) at temperature, T≈80 ∘C and effective pressure, Peff=50 MPa, during which we collected mechanical, acoustic and pore fluid chemistry data. We observed transient creep at stresses as low as 11 % of the failure strength. Acoustic emissions (AEs) correlated strongly with strain accumulation, indicating that the creep deformation was a brittle process in agreement with microstructural observations. The rate and magnitude of AEs were higher in fluid-saturated experiments than in dry conditions. We infer that the predominant mechanism governing creep deformation is time- and stress-dependent subcritical dilatant cracking. Our results suggest that the presence of aqueous fluids exerts first-order control on creep deformation of basaltic rocks, while the composition of the fluids plays only a secondary role under the studied conditions.