In 2013, the Pacific Northwest National Laboratory led a geologic carbon sequestration field demonstration where ∼1000 tonnes of CO 2 was injected into several deep Columbia River Basalt zones near Wallula, Washington. Rock core samples extracted from the injection zone two years after CO 2 injection revealed nascent carbonate mineralization that was qualitatively consistent with expectations from laboratory experiments and reactive transport modeling. Here, we report on a new detailed analysis of the 2012 pre-injection and 2015 post-injection hydrologic tests that capitalizes on the difference in fluid properties between scCO 2 and water to assess changes in near-field, wellbore, and reservoir conditions that are apparent approximately two years following the end of injection. This comparative hydrologic test analysis method provides a new way to quantify the amount of injected CO 2 that was mineralized in the field test. Modeling results indicate that approximately 60% of the injected CO 2 was sequestered via mineralization within two years, with the resulting carbonates occupying ∼4% of the available reservoir pore space. The method presented here provides a new monitoring tool to assess the fate of CO 2 injected into chemically reactive basalt formations but could also be adapted for long-term monitoring and verification within more traditional subsurface carbon storage reservoirs.

PrefaceThis STOMP (Subsurface Transport Over Multiple Phases) guide document describes the theory, use, and application of the STOMP-CO2 and STOMP-CO2e operational modes. These operational modes of the STOMP simulator are configured to solve problems involving the geologic sequestration of CO2 in saline reservoirs. STOMP-CO2 is the isothermal version and STOMP-CO2e is the nonisothermal version. These core operational modes solve the governing conservation equations for component flow and transport through geologic media; where, the STOMP-CO2 components are water, CO2 and salt and the STOMPCO2e operational mode also includes an energy conservation equation. Geochemistry can be included in the problem solution via the ECKEChem (Equilibrium-Conservation-Kinetic-Equation Chemistry) module, and geomechanics via the EPRMech (Elastic-Plastic-Rock Mechanics) module. This addendum is designed to provide the new user with a full guide for the core capabilities of the STOMP-CO2 and -CO2e simulators, and to provide the experienced user with a quick reference on implementing features. Several benchmark problems are provided in this addendum, which serve as starting points for developing inputs for more complex problems and as demonstrations of the simulator's capabilities.STOMP-CO2 and -CO2e are written in Fortran 90 with dynamic memory allocation. The codes can be configured for either a banded or conjugate gradient linear system solver. The simulators are provided as source code to encourage the open exchange of scientific and mathematical ideas, but this requires that the user compile and link the code into an executable. In writing this addendum the authors have assumed that the reader is familiar with numerical simulation of multifluid subsurface flow and reactive transport and with the computing environment on which they plan to compile and execute the STOMP-CO2 and -CO2e simulators. The simulator is maintained following a configuration management plan as a collection of source code files. Assembly of the library files into a single source code or executable occurs through a software maintenance utility. Version numbers are assigned to individual files in the STOMP library of files and those version numbers are reported to standard output and the "output" file for the active files in the executable at the conclusion of the execution. The memory requirements for executing the STOMP-CO2 and -CO2e simulators are dependent on the complexity of the physical system to be modeled and the size and dimensionality of the computational domain. Likewise, execution speed depends on the problem complexity, size and dimensionality of the computational domain, and computer performance. v SummaryGeologic sequestration is currently being practiced and scientifically evaluated as a critical component in a broad strategy, comprising new practices and technologies, for mitigating global climate change due to anthropogenic emissions of CO2. Demonstrating that geologic sequestration of CO2 is safe and effective, and gaining public acceptance...

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Injecting supercritical CO2 (scCO2) into basalt formations for long-term storage is a promising strategy for mitigating CO2 emissions. Mineral carbonation can result in permanent entrapment of CO2; however, carbonation kinetics in thin H2O films in humidified scCO2 is not well understood. We investigated forsterite (Mg2SiO4) carbonation to magnesite (MgCO3) via amorphous magnesium carbonate (AMC; MgCO3·xH2O, 0.5 < x < 1), with the goal to establish the fundamental controls on magnesite growth rates at low H2O activity and temperature. Experiments were conducted at 25, 40, and 50 °C in 90 bar CO2 with a H2O film thickness on forsterite that averaged 1.78 ± 0.05 monolayers. In situ infrared spectroscopy was used to monitor forsterite dissolution and the growth of AMC, magnesite, and amorphous SiO2 as a function of time. Geochemical kinetic modeling showed that magnesite was supersaturated by 2 to 3 orders of magnitude and grew according to a zero-order rate law. The results indicate that the main drivers for magnesite growth are sustained high supersaturation coupled with low H2O activity, a combination of thermodynamic conditions not attainable in bulk aqueous solution. This improved understanding of reaction kinetics can inform subsurface reactive transport models for better predictions of CO2 fate and transport.