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We found that supercritical CO2 and the availability of protein-rich matter in depleted oil reservoirs can result in the biogenic production of H2 from oil hydrocarbons by indigenous microbial communities. Our experimental results support the hypothesis that a decrease in pH to acidic levels due to the dissolution of supercritical CO2 into the formation water and availability of protein-rich matter favors the activity of H2-producing microbial communities over the activity of H2-using microbial communities. To determine where, when, and how much H2 could be produced in a depleted oil reservoir injected with CO2 and produced water (PW) supplied with protein-rich matter, we simulated the biogenic production of H2 for the Morrow B sandstone reservoir. Simulations were conducted using CO2Bio, a program developed to simulate the multiphase bio-geochemical reactive transport of CO2-CH4-H2-H2S gases in geological carbon storage (GCS) sites. The microbiological capabilities of CO2Bio are validated against batch reaction experimental results. Our field-scale simulation results indicate that 154 – 1673 kg of H2 could be produced after 100 days of CO2 and PW co-injection into a single well of radial flow, and that sandstone reservoirs are more suitable than carbonate reservoirs to produce H2 from dissolved hydrocarbons. Based on the obtained experimental and simulation results, we propose a new H2 production method that couples GCS and PW disposal in depleted oil reservoirs to attenuate environmental and energy issues related to global warming derived from atmospheric pollution with CO2, risk of freshwater resources contamination with PW, and depletion of energy resources. 

Pore-scale modeling is essential in understanding and predicting flow and transport properties of rocks. Generally, pore-scale modeling is dependent on imaging technologies such as Micro Computed Tomography (micro-CT), which provides visual confirmation into the pore microstructures of rocks at a representative scale. However, this technique is limited in the ability to provide high resolution images showing the pore-throats connecting pore bodies. Pore scale simulations of flow and transport properties of rocks are generally done on a single 3D pore microstructure image. As such, the simulated properties are only representative of the simulated pore-scale rock volume. These are the technological and computational limitations which we address here by using a stochastic pore-scale simulation approach. This approach consists of constructing hundreds of 3D pore microstructures of the same pore size distribution and overall porosity but different pore connectivity. The construction of the 3D pore microstructures incorporates the use of Mercury Injection Capillary Pressure (MICP) data to account for pore throat size distribution, and micro-CT images to account for pore body size distribution. The approach requires a small micro-CT image volume (7–19 mm3) to reveal key pore microstructural features that control flow and transport properties of highly heterogeneous rocks at the core-scale. Four carbonate rock samples were used to test the proposed approach. Permeability calculations from the introduced approach were validated by comparing laboratory measured permeability of rock cores and permeability estimated using five well-known core-scale empirical model equations. The results show that accounting for the stochastic connectivity of pores results in a probabilistic distribution of flow properties which can be used to upscale pore-scale simulated flow properties to the core-scale. The use of the introduced stochastic pore-scale simulation approach is more beneficial when there is a higher degree of heterogeneity in pore size distribution. This is shown to be the case with permeability and hydraulic tortuosity which are key controls of flow and transport processes in rocks. 

Alkalinity is a critical parameter for describing the composition, pH buffer capacity, and precipitation potential of petroleum produced water (PW). Besides salinity, alkalinity and metal concentrations are generally greater in PW than in freshwater (FW) and seawater. This study presents batch reaction experimental and simulation results showing that the removal of Ba, Sr, and Cd from PW by dolomite is mostly due to sorption reactions, with sorption reactions and thus removal levels being higher for Cd than for Ba and Sr. In contrast, we found that the removal of Pb and As from PW by dolomite is largely due to precipitation and coprecipitation reactions of carbonate minerals on dolomite. Analyses of changes in the morphology as well as in the elemental and mineral composition of dolomite surface, along with pH, alkalinity, and Ba, Sr, Cd, Pb, and As removal measurements using synthetic PW and FW containing high concentrations (∼100 mg/L) of single and mixture toxic metals and metalloids (Ba, Sr, Cd, Pb, and As) at different initial alkalinity and pH conditions, indicate that in addition to salinity, alkalinity and pH generated from the dissolution of dolomite controls the removal of Ba, Sr, Cd, Pb, and As from PW by dolomite. However, we found that their impact is different for each metal in PW and FW. Ba, Sr, and Cd removal by dolomite is 10, 2, and 4 times smaller in PW than in freshwater (FW), respectively. Whereas As removal is practically the same regardless of salinity. Moreover, this study reveals the need of thermodynamic data of complex carbonate minerals formed from the precipitation of Ba, Sr, Cd, Pb, and As to capture the effect of alkalinity on their removal from PW by dolomite. 

Predicting the transport of toxic metals in dolomite saline aquifers where petroleum produced water (PW) is commonly injected is important to prevent underground sources of drinking water contamination. This study presents new experimental results on the degree and impact of precipitation and sorption reactions on the transport of high concentrations of toxic metals (80-100 mg-Ba/L, 80-100 mg-Sr/L, 70-100 mg-Cd/L, 2-100 mg-Pb/L, and 80-100 mg-As/L) in dolomite injected with PW of variable alkalinity (0–200 mg/L), total dissolved solids (1700–77,000 mg/L), and pH (2–7). Changes in the elemental and mineral composition of dolomite surface were measured by BSEs SEM, SEM-EDS, and high-resolution XRD analyses. The results reveal a key role of alkalinity generated from the dissolution of dolomite. We show that a short initial stage where the removal of toxic metals is driven by the initial pH and alkalinity of PW is followed by a prolonged stage where the removal of toxic metals by sorption and precipitation reactions is driven by the alkalinity and pH that results from the kinetic dissolution of dolomite. Precipitated/coprecipitated metals were carbonate minerals reflecting the metal composition of PW. Attained removal levels of tested toxic metals from 1 L of PW using a dolomite core made of 200 g were >90% for Pb, >50% for As, >30% for Cd, and >5% for Ba and Sr. Apparently, the in-situ generation of alkalinity (carbonate ions) and sorption reactions of metals on dolomite catalyzes the precipitation of toxic metals as carbonate minerals. This catalytic effect of dolomite is different with PW and fresh water (FW) of low salinity (NaCl). Precipitation reactions are more prominent with FW than with PW, whereas sorption reactions are more prominent with PW than with FW.