Predictive surface complexation model of the calcite-aqueous solution interface: the impact of high concentration and complex composition of brines

• Published in: Journal of Colloid and Interface Science
• Main Authors: Vinogradov, Jan, Hidayat, Miftah, Sarmadivaleh, Mohammad, Derksen, Jos, Vega-Maza, David, Iglauer, Stefan, Jougnot, Damien, Azaroual, Mohamed, Leroy, Philippe
• Other Authors: University of Aberdeen, Milieux Environnementaux, Transferts et Interactions dans les hydrosystèmes et les Sols (METIS), École pratique des hautes études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences de la Terre d'Orléans - UMR7327 (ISTO), Bureau de Recherches Géologiques et Minières (BRGM) (BRGM)-Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS), Milieux Poreux - UMR7327, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Bureau de Recherches Géologiques et Minières (BRGM) (BRGM)-Observatoire des Sciences de l'Univers en région Centre (OSUC), Bureau de Recherches Géologiques et Minières (BRGM) (BRGM), O-ZNS project which is part of PIVOTS project (financial support provided by the Région Centre-Val de Loire and the French Ministry of Higher Education and Research).
• Format: Article in Journal/Newspaper
• Language: English
• Published: HAL CCSD 2022
• Subjects: zeta potential; calcite; aqueous solutions; surface complexation model; high salinity; complex composition; predictive model Stern layer capacitance; [SDU]Sciences of the Universe [physics]; Iceland
• Online Access: https://hal-insu.archives-ouvertes.fr/insu-03439388; https://hal-insu.archives-ouvertes.fr/insu-03439388/document; https://hal-insu.archives-ouvertes.fr/insu-03439388/file/1-s2.0-S0021979721019925-main.pdf; https://doi.org/10.1016/j.jcis.2021.11.084

International audience Electrochemical interactions at calcite-water interface are characterized by the zeta potential and play an important role in many subsurface applications. In this work we report a new physically meaningful surface complexation model that is proven to be efficient in predicting calcite-water zeta potentials for a wide range of experimental conditions.Our model uses a two-stage optimization for matching experimental observations. First, equilibrium constants are optimized, and the Stern layer capacitance is optimized in the second stage. The model is applied to a variety of experimental sets that correspond to intact natural limestones saturated with equilibrated solutions of low-to-high salinity, and crushed Iceland Spar sample saturated with NaCl at non-equilibrium conditions.The proposed linear correlation of the Stern layer capacitance with the ionic strength is the main novel contribution to our surface complexation model without which high salinity experiments cannot be modelled. Our model is fully predictive given accurately known conditions. Therefore, the reported parameters and modelling protocol are of significant importance for improving our understanding of the complex calcite-water interfacial interactions. The findings provide a robust tool to predict electrochemical properties of calcite-water interfaces, which are essential for many subsurface applications including hydrology, geothermal resources, CO2 sequestration and hydrocarbon recovery.