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In order to investigate the interphase mass transfer and component distribution characteristics of the CO2-water system under micro-scale and nano-scale transport conditions, a micro-scale kinetic model representing interphase mass transfer in the CO2-water/saline system is developed in this paper. The molecular dynamics method is employed to delineate the diffusion and mass transfer processes of the system's components, revealing the extent of the effects of variations in temperature, pressure, and salt ion concentration on interphase mass transfer and component distribution characteristics. The interphase mass transfer process in the CO2-water system under transport conditions can be categorized into three stages: approach, adsorption, and entrance. As the system temperature rises and pressure decreases, the peak density of CO2 molecules at the gas-liquid interface markedly drops, with their aggregation reducing and their diffusion capability enhancing. The specific hydration structures between salt ions and water molecules hinder the entry of CO2 into the aqueous phase. Additionally, as the salt concentration in water increases, the density peak of CO2 molecules at the gas-liquid interface slightly increases, while the density value in the water phase region significantly decreases.

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Thermal enhanced soil vapour extraction (T-SVE) is a remedial technique involving gas, aqueous, solid and nonaqueous phases along with mass and heat transfer. Interphase mass transfer of contaminants and water evaporation/condensation will cause the redistribution of phase saturation, eventually affecting the performance of T-SVE. In this study, a multiphase, multicompositional and nonisothermal model was developed to simulate the T-SVE treatment of contaminated soil. The model was calibrated using published data from the SVE laboratory and T-SVE field experiments. The temporal and spatial distributions of the contaminant concentrations in the four different phases, the mass transfer rates and the temperatures are presented to reveal the coupling interactions that occur between multiple fields during T-SVE. A series of parametric studies were carried out to investigate the effect of water evaporation and adsorbed/dissolved contaminants on the T-SVE performance. It was found that endothermic evaporation, exothermic condensation and the interaction between different removal paths of a contaminant played critical roles in the thermal enhancement of SVE. Ignoring them can result in significant differences in the removal efficiency values.

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Release of benzene, toluene, ethylbenzene, and xylene (BTEX) as components of the light non-aqueous phase liquids (LNAPL) contaminates soil and groundwater. Assessing the mechanisms of degradation and mineralization of BTEX in groundwater helps understand the migration of the dissolved plume, enabling the reduction of risks to humans. Here, we studied the fate of ethylbezene, m,p-xylenes and o-xylenes and the accompanying formation of methane in a Cenozoic lateritic aquifer in Brazil by compound-specific carbon stable isotope analysis (CSIA), to gain insights into the complex dynamics of release and biodegradation of BTEX in the LNAPL source zone. The enrichment of ∂13C in aromatic compounds dissolved in groundwater compared to the corresponding compounds in LNAPL indicate that CSIA can provide valuable information regarding biodegradation. The isotopic analysis of methane provides direct indication of oxidation mediated by aquifer oxygenation. The ∂13C-CO2 values indicate methanogenesis prevailing at the border and aerobic biodegradation in the center of the LNAPL source zone. Importantly, the isotopic results allowed major improvements in the previously developed conceptual model, supporting the existence of oxic and anoxic environments within the LNAPL source zone.

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Practical designs of non-aqueous phase liquids (NAPLs) remediation strategies require reliable modeling of interphase mass transfer to predict the retraction of NAPL during processes such as dissolution. In this work, the dissolution process of NAPL during two-phase flow in heterogeneous porous media is studied using pore-network modeling and micromodel experiments. A new physical-experimental approach is proposed to enhance the prediction of the dissolution process during modeling of interphase mass transfer. In this regard, the normalized average resident solute concentration is evaluated for describing the dissolution process at pore-level. To incorporate the effect of medium heterogeneities, a new experimental factor is considered for enhancing corner diffusion modeling. In addition, capillary desaturation curves (CDCs) are predicted during hydraulic flow modeling to estimate initial residual NAPL saturation. The developed network model can predict residual NAPL saturations and mass transfer rate coefficient for a NAPL-water system at different injection rates and fluid saturations. The evaluated mass transfer rate coefficients using the proposed physical-experimental approach show a significant improvement compared to either mechanistic or empirical methods. The proposed approach in this study can be attractive for possible applications in commercial simulators of contaminant transport in porous media.

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Multiphase flow modeling is often used for the comparison and optimization of subsurface nonaqueous phase liquid (NAPL) remediation schemes. The calibration of such models is a challenging task due to the lack of detailed data describing the initial NAPL spatial distribution and the processes governing the fate and transport of NAPLs in porous media. In this study laboratory scale experiments were conducted to evaluate reagent-enhanced dense nonaqueous phase liquid (DNAPL) solubilization in saturated heterogeneous media. The DNAPL consisted of both pooled and residual saturation forms. To gain insight into the influence of various input parameters on effluent concentrations, the multiphase flow program was used to compute the sensitivity coefficients of key parameters, relating to the flow, flushing solution properties, soil parameters, NAPL distribution and mass transfer coefficient. The sensitivity coefficients were, in turn, used to aid in the model calibration and to underline the difficulties associated with the calibration of multiphase flow models, most notably the non-uniqueness of the calibration process when complete information is lacking. To alleviate this uncertainty and provide additional constraints, the conducted flushing experiments were jointly used to calibrate the multiphase flow model. The results of the model calibration suggest that the interphase mass transfer coefficient is dependent on the properties of the reagent aqueous solution used for DNAPL remediation, most notably the viscosity and interfacial tension.

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The rate of interphase mass transfer from non-aqueous phase liquids (NAPLs) entrapped in the subsurface into the surrounding mobile aqueous phase is commonly expressed in terms of Sherwood (Sh) correlations that are expressed as a function of flow and porous media properties. Because of the lack of precise methods for the estimation of the interfacial area separating the NAPL and aqueous phases, most studies have opted to use modified Sherwood expressions that lump the interfacial area into the interphase mass transfer coefficient. To date, there are only two studies in the literature that have developed non-lumped Sherwood correlations; however, these correlations have undergone limited validation. In this paper controlled dissolution experiments from pooled NAPL were conducted. The immobile NAPL mass is placed at the bottom of a flow cell filled with porous media with water flowing horizontally on top. Effluent aqueous phase concentrations were measured for a wide range of aqueous phase velocities and for two different porous media. To interpret the experimental results, a two-dimensional pore network model of the NAPL dissolution kinetics and aqueous phase transport was developed. The observed effluent concentrations were then used to compute best-fit mass transfer coefficients. Comparison of the effluent concentrations computed with the two-dimensional pore network model to those estimated with one-dimensional analytical solutions indicates that the analytical model which ignores the transport in the lateral direction can lead to under-estimation of the mass transfer coefficient. Based on system parameters and the estimated mass transfer coefficients, non-lumped Sherwood correlations were developed and compared to previously published data. The developed correlations, which are a significant improvement over currently available correlations that are associated with large uncertainties, can be incorporated into future modeling studies requiring non-lumped Sh expressions.

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