The impact of ionic association with the carbonate surface and its influence toward carbonate wettability remains unclear and is an important topic of interest in the current literature. In this work, a triple layer model (TLM) approach was used to capture the electrokinetic interactions at both calcite–brine and oil–brine interfaces. The developed TLM was assembled against measured ζ-potential values from the literature, successfully capturing the trends and closely matching the ζ-potential magnitudes. The developed TLM was compared to a diffused layer model (DLM) presented in previous works, with the DLM showing a better match to the ζ-potential values for seawater brine solutions. The ζ-potential values predicted from both surface complexation models (SCMs) were used to calculate the total interaction energy (or potential) based on the Derjaguin, Landau, Verwey, and Overbeek (DLVO) theory. It was observed that low Mg2+ and high SO42– concentrations in modified composition brine (MCB) made the calcite–brine interface more negative. However, at the oil–brine interface, low Mg2+ made the oil–brine interface more negative but high SO42– concentrations slightly shifted the oil–brine ζ-potential toward negative. At the crude oil–brine–rock (COBR) interfaces, low Mg2+ and high SO42– concentrations in the MCB were observed to generate a greater repulsive interaction energy, which could trigger carbonate wettability alteration toward water wetness. The absolute sum of the ζ-potential at both interfaces was observed to be correlated to the total interaction potential at a 0.25 nm separating distance. Thus, an increase in the absolute sum of the ζ-potentials would generate a greater repulsive interaction potential and trigger wettability alteration. Therefore, these SCMs can be applied to design modified composition brine capable of triggering a repulsive interaction energy to alter carbonate wettability toward water wetness.

https://kuscholarworks.ku.edu/bitstream/1808/32738/1/Tetteh_2022.pdf

Ionic Interactions at the Crude Oil–Brine–Rock Interfaces Using Different Surface Complexation Models and DLVO Theory: Application to Carbonate Wettability

The effects of CO2-water-rock interactions on the injectivity and safety of CO2 geological storage have drawn wide attention. The geochemical reaction mechanisms in carbonate formations after CO2 injection are still controversial. To better understand the transformation of injected CO2 in carbonates and the involved geochemical reactions, we first conducted autoclave experiments reproducing the in-situ conditions of the Lianglitage Formation, Yingshan Formation, and Qiulitage Formation at the Tazhong Uplift in the Tarim Basin. We then established a batch model using TOUGHREACT-ECO2H, validated with the experimental results, to simulate the long-term CO2-water-rock interactions. It was found that the initial mineral compositions and water chemistry have important effects on the CO2-water-rock interactions in carbonate formations. The experiment results show that the dissolution of calcite and dolomite dominates in the early reaction period. However, we still observed some secondary minerals, such as ankerite, montmorillonite, calcite, and dolomite. The CO2-water-rock reactions can be more dramatic when the contents of calcite and dolomite in carbonates are closer. Moreover, the long-term simulation results show that calcite, magnesite, and hematite are the main formed secondary minerals, whereas dolomite is the major dissolved mineral. This study is helpful for a better understanding of the CO2 mineral trapping mechanism in carbonate formations.

https://www.mdpi.com/2075-163X/12/5/635/pdf?version=1652782910

CO2-Water-Rock Interactions in Carbonate Formations at the Tazhong Uplift, Tarim Basin, China

Carbonate reservoirs are made up of predominantly calcite and dolomite minerals and hold significant hydrocarbon reserves globally. However, the production from carbonate reservoirs is limited due to their wettability, which controls the production and fluid distribution. To develop efficient strategies for producing from these formations, it is necessary to understand the underlining mechanisms of carbonate rock wettability. We believe that understanding the native state of the rock mineral in the reservoir environment and how oilfield operations affect the wetting state of minerals is critical to demystifying the change in carbonate rock wettability. Thus, this study extends the understanding of the surface charge development of calcite minerals and provides useful insight into the mineral’s surface charge development. Zeta potential measurements and molecular dynamics (MD) simulations of calcite in different fluids of varying composition and salinity were investigated. We have considered both the mixed brine (seawater and reservoir water) and individual salt brine (i.e., NaCl, MgCl2, and CaCl2). The results show that the calcite mineral surface charge is controlled by the composition and salinity of the surrounding fluids. Indeed, we found that monovalent ions have dominant contributions to the total calcite surface charge. The adsorptions of Na+ and Cl– shape the stern layer structure in the first two calcite hydration monolayers. We found that the interplay between the calcite surface affinity to the brine ions and the hydration-free energies are the two critical parameters shaping the final mineral surface charge. We believe that our study provides essential atomic insights into the calcite–brine interfaces and how ions interact with the surface to control the surface charge, which are vital to the quest for wettability control. 

Calcite–Brine Interface and Its Implications in Oilfield Applications: Insights from Zeta Potential Experiments and Molecular Dynamics Simulations

Recently, the application of low salinity water (LSW), nanoparticles (NPs), and surfactants (collectively abbreviated as LNS) in carbonate formations for enhanced oil recovery (EOR) purposes has been under investigation, but relatively few studies have been performed for their implementation in fractured carbonate reservoirs (FCRs). The objective of this study is to apply the recently proposed method of alternatively injecting LNS in cycles into FCRs using silica and zirconia NPs. The cumulative oil recovered from the two coreflooding experiments performed at 3000 psi overburden pressure and 70 °C temperature is reported in this study in addition to spontaneous imbibition (SI) experiments. The experimental design is structured to depict the best industrial practice for the injected fluids in FCRs. Furthermore, this work investigates the effect of zirconia NPs on the interfacial tension (IFT) between the injected fluids and crude oil under the previously stated experimental conditions. The outcome of these experiments divulges that the alternating injection of LNS employing silica and zirconia NPs is effective and well suited for EOR applications in FCRs owing to a cumulative oil recovery of approximately 8 and 7% of the original oil in place (OOIP), respectively. This study validates the implementation of the recently proposed alternating injection of the LNS technique for FCRs and shows its performance utilizing newly acquired zirconia NPs, which is relevant for industrial application at a large scale. 

Experimental Study on Alternating Injection of Silica and Zirconia Nanoparticles with Low Salinity Water and Surfactant into Fractured Carbonate Reservoirs for Enhanced Oil Recovery

/pdf/low-salinity-water-and-polymer-flooding-in-sandstone-11i0dz8t.pdf

Low salinity water and polymer flooding in sandstone reservoirs: Upscaling from nano-to macro-scale using the maximum energy barrier

Geochemical Feasibility of Brine Exchange Between Arbuckle and Lansing-Kansas City Formations as a Produced Water Management Alternative

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Ionic Interactions at the Crude Oil–Brine–Rock Interfaces Using Different Surface Complexation Models and DLVO Theory: Application to Carbonate Wettability

Geochemical Feasibility of Brine Exchange Between Arbuckle and Lansing-Kansas City Formations as a Produced Water Management Alternative