Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept

Reactive transport modeling is an important tool for the analysis of coupled physical, chemical, and biological processes in Earth systems. Observed reactive transport in heterogeneous porous media shows a different behavior than the established transport laws for homogeneous media. Natural aquifers...

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Autor: Perez Fonseca, Lazaro J.
Tipo de recurso: tesis doctoral
Fecha de publicación:2019
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/176425
Acceso en línea:https://hdl.handle.net/2117/176425
https://dx.doi.org/10.5821/dissertation-2117-176425
Access Level:acceso abierto
Palabra clave:Àrees temàtiques de la UPC::Enginyeria civil
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dc.title.none.fl_str_mv Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
title Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
spellingShingle Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
Perez Fonseca, Lazaro J.
Àrees temàtiques de la UPC::Enginyeria civil
title_short Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
title_full Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
title_fullStr Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
title_full_unstemmed Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
title_sort Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella concept
dc.creator.none.fl_str_mv Perez Fonseca, Lazaro J.
author Perez Fonseca, Lazaro J.
author_facet Perez Fonseca, Lazaro J.
author_role author
dc.contributor.none.fl_str_mv Dentz, Marco
Hidalgo González, Juan J.
dc.subject.none.fl_str_mv Àrees temàtiques de la UPC::Enginyeria civil
topic Àrees temàtiques de la UPC::Enginyeria civil
description Reactive transport modeling is an important tool for the analysis of coupled physical, chemical, and biological processes in Earth systems. Observed reactive transport in heterogeneous porous media shows a different behavior than the established transport laws for homogeneous media. Natural aquifers exhibit physical and chemical heterogeneities at all scales, which leads to reaction and transport dynamics that cannot be explained by traditional reactive models based on the advection-dispersion-reaction equation (ADRE). In particular, the discrepancy is traced back to the nonuniform nature of flow velocity fields, complex spatial concentration distributions, and the degree of mixing between reactants. The role and contribution of these factors is key to provide accurate predictions of reactions. The complexity of the task lies in the enormous range of spatial and temporal scales that reactants find in natural porous media. Hence, the complete characterization of the fate of chemical reactions requires that models accounts for the basic mechanisms that govern the mixing and reaction dynamics. In this thesis, we present a novel methodology for the simulation of homogeneous chemical reactions. The proposed methodology is a random walk particle tracking approach (RWPT) coupled with reactions that simulates bimolecular chemical reactions, and is equivalent to the ADRE. Reactions among particles are determined by a reaction probability given in terms of the reaction rate coefficient, the total number of particles, and an interaction radius that describes a well-mixed support volume at which all particles have the same probability to react. The method is meshless and free of numerical dispersion. The RWPT approach is validated against analytical solutions for different flow scenarios under slow and fast reaction kinetics. We focus on the impact of the mixing degree between chemical species and its role in the global reaction behavior. We first consider a reactive displacement in a Poiseuille flow through a pore channel, this system allow us to quantify the impact of the interaction of interface deformation and diffusion on mixing and reactive transport. We observe overestimation of the global reaction efficiency by the use of the Taylor dispersion coefficient at preasymptotic times, when the system is characterized by incomplete mixing. Next, we observe features of incomplete mixing in a synthetic porous medium. Results show that macroscopic predictions using the hydrodynamic dispersion coefficient overestimates the amount of reaction. In addition, we analize the bimolecular reactive transport in a laboratory experiment, where we find that the amount of reaction is affected by the amount of mixing due to difusion, the amount of mixing due to spreading and the degree of heterogeneity of the flow field. The contributions of these factors induces that ADRE estimation of the total reaction product fails. In order to characterize incomplete mixing and provide an explicit relation between fluid deformation and its impact on the temporal evolution of the chemical reactivity, we develop the dispersive lamella approach based on the concept of effective dispersion which accurately predicts the full evolution of the product mass. Specifically, the approach captures the impact of interface deformation and diffusive coalescence. Using this methodology, we quantify the impact of flow heterogeneities on the amount of fluid mixing in a pore channel, where we observe three temporal regimes based on the production rate of the product mass. In addition, the dispersive lamella predictions capture the kinetics of the reaction in a synthetic porous medium. Results reveal that reaction behavior is controlled by the interface front between the two reactants. In the pore-scale experimental visualization, the dispersive lamella show that reaction is controlled by the deformed mixing interface at early times, and for fingering coalescence at late times.
publishDate 2019
dc.date.none.fl_str_mv 2019
2019-05-17
2020
2020-02-03
dc.type.none.fl_str_mv doctoral thesis
http://purl.org/coar/resource_type/c_db06
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/doctoralThesis
format doctoralThesis
dc.identifier.none.fl_str_mv https://hdl.handle.net/2117/176425
https://dx.doi.org/10.5821/dissertation-2117-176425
url https://hdl.handle.net/2117/176425
https://dx.doi.org/10.5821/dissertation-2117-176425
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2

http://creativecommons.org/licenses/by-nd/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
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eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Universitat Politècnica de Catalunya
publisher.none.fl_str_mv Universitat Politècnica de Catalunya
dc.source.none.fl_str_mv reponame:UPCommons. Portal del coneixement obert de la UPC
instname:Universitat Politècnica de Catalunya (UPC)
instname_str Universitat Politècnica de Catalunya (UPC)
reponame_str UPCommons. Portal del coneixement obert de la UPC
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spelling Upscaling mixing-limited chemical reactions from pore to continuum scale using the dispersive lamella conceptPerez Fonseca, Lazaro J.Àrees temàtiques de la UPC::Enginyeria civilReactive transport modeling is an important tool for the analysis of coupled physical, chemical, and biological processes in Earth systems. Observed reactive transport in heterogeneous porous media shows a different behavior than the established transport laws for homogeneous media. Natural aquifers exhibit physical and chemical heterogeneities at all scales, which leads to reaction and transport dynamics that cannot be explained by traditional reactive models based on the advection-dispersion-reaction equation (ADRE). In particular, the discrepancy is traced back to the nonuniform nature of flow velocity fields, complex spatial concentration distributions, and the degree of mixing between reactants. The role and contribution of these factors is key to provide accurate predictions of reactions. The complexity of the task lies in the enormous range of spatial and temporal scales that reactants find in natural porous media. Hence, the complete characterization of the fate of chemical reactions requires that models accounts for the basic mechanisms that govern the mixing and reaction dynamics. In this thesis, we present a novel methodology for the simulation of homogeneous chemical reactions. The proposed methodology is a random walk particle tracking approach (RWPT) coupled with reactions that simulates bimolecular chemical reactions, and is equivalent to the ADRE. Reactions among particles are determined by a reaction probability given in terms of the reaction rate coefficient, the total number of particles, and an interaction radius that describes a well-mixed support volume at which all particles have the same probability to react. The method is meshless and free of numerical dispersion. The RWPT approach is validated against analytical solutions for different flow scenarios under slow and fast reaction kinetics. We focus on the impact of the mixing degree between chemical species and its role in the global reaction behavior. We first consider a reactive displacement in a Poiseuille flow through a pore channel, this system allow us to quantify the impact of the interaction of interface deformation and diffusion on mixing and reactive transport. We observe overestimation of the global reaction efficiency by the use of the Taylor dispersion coefficient at preasymptotic times, when the system is characterized by incomplete mixing. Next, we observe features of incomplete mixing in a synthetic porous medium. Results show that macroscopic predictions using the hydrodynamic dispersion coefficient overestimates the amount of reaction. In addition, we analize the bimolecular reactive transport in a laboratory experiment, where we find that the amount of reaction is affected by the amount of mixing due to difusion, the amount of mixing due to spreading and the degree of heterogeneity of the flow field. The contributions of these factors induces that ADRE estimation of the total reaction product fails. In order to characterize incomplete mixing and provide an explicit relation between fluid deformation and its impact on the temporal evolution of the chemical reactivity, we develop the dispersive lamella approach based on the concept of effective dispersion which accurately predicts the full evolution of the product mass. Specifically, the approach captures the impact of interface deformation and diffusive coalescence. Using this methodology, we quantify the impact of flow heterogeneities on the amount of fluid mixing in a pore channel, where we observe three temporal regimes based on the production rate of the product mass. In addition, the dispersive lamella predictions capture the kinetics of the reaction in a synthetic porous medium. Results reveal that reaction behavior is controlled by the interface front between the two reactants. In the pore-scale experimental visualization, the dispersive lamella show that reaction is controlled by the deformed mixing interface at early times, and for fingering coalescence at late times.Los modelos de transporte reactivo son una herramienta importante para el análisis de procesos físicos y químicos en los sistemas terrestres. Los procesos de transporte reactivo observados en medios porosos heterogéneos muestran un comportamiento diferente al de las leyes de transporte para medios homogéneos. Los acuíferos exhiben heterogeneidades a todas las escalas, lo que lleva a dinámicas de transporte y reacción que no pueden explicarse mediante modelos de transporte reactivo tradicionales basados en la ecuación advocación-dispersión-reacción (ADRE). La discrepancia de este comportamiento se remonta a la naturaleza no uniforme de los campos de velocidad de flujo, a complejas distribuciones de concentración y al grado de mezcla entre los reactivos. La contribución de estos factores es clave para proporcionar predicciones precisas de las reacciones químicas. Por lo tanto, la caracterización completa de las reacciones químicas requiere que los modelos determinen los mecanismos básicos que gobiernan la dinámica de mezcla y reacción. En esta tesis, presentamos una metodología para la simulación de reacciones químicas. La metodología propuesta es un “random walk particle tracking” (RWPT) acoplado a reacciones que simula reacciones químicas bimoleculares, y es equivalente a la ADRE. Las reacciones entre partículas están determinadas por una probabilidad de reacción basada en el coeficiente de velocidad de reacción, el número total de partículas y el radio de interacción que describe un volumen de mezcla completa en el que todas las partículas tienen la misma probabilidad de reaccionar. El RWPT se valida frente a soluciones analíticas para diferentes escenarios de flujo con cinéticas lentas y rápidas. Además, estudiamos el impacto del grado de mezcla entre las diferentes especies químicas y su papel en el comportamiento global de la reacción. Primero consideramos un desplazamiento reactivo en un flujo de Poiseuille a través de un canal de poro. Y observamos la sobreestimación de la eficiencia global de reacción mediante el uso del coeficiente de dispersión de Taylor en tiempos preasintoticos. Observamos el grado de mezcla de los reactivos en un medio poroso sintético. Los resultados muestran que las predicciones macroscópicas que utilizan el coeficiente de dispersión hidrodinámica sobreestiman la cantidad de reacción. Además, analizamos el transporte reactivo en un experimento de laboratorio, donde encontramos que la cantidad de reacción se ve afectada por la cantidad de mezcla debida a la difusión, la cantidad de mezcla debida a la extensión de la interfaz y el grado de heterogeneidad del campo de flujo. La contribución de estos factores induce que la estimación de la masa total del producto de reacción por parte de la ADRE falle. Para caracterizar la mezcla incompleta y proporcionar una relación explicita entre la deformación del fluido y su impacto en la evolución temporal de la reactividad química, desarrollamos el método de la lamela dispersiva basado en el concepto de dispersión efectiva que predice con precisión la evolución de la masa total del producto de la reacción. El método capta el impacto de la deformación de la interfaz y la coalescencia difusiva. Usando esta metodología, cuantificamos el impacto de las heterogeneidades de flujo en el grado de mezcla de reactivos en un canal de poro, donde observamos tres regímenes temporales basados en la tasa de producción de la masa del producto. La predicción de las lamelas dispersivas captura la cinética de la reacción en el medio poroso sintético estudiado. Los resultados revelan que la reacción está controlada por la interfaz de mezcla entre los reactivos. En la visualización experimental a escala de poro, los resultados de las lamelas dispersivas muestran que la reacción está controlada por la interfaz de mezcla deformada en los primeros tiempos, y para la fusión de la digitación en los últimos tiempos.Universitat Politècnica de CatalunyaDentz, MarcoHidalgo González, Juan J.20192019-05-1720202020-02-03doctoral thesishttp://purl.org/coar/resource_type/c_db06VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/doctoralThesisapplication/pdfhttps://hdl.handle.net/2117/176425https://dx.doi.org/10.5821/dissertation-2117-176425reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2http://creativecommons.org/licenses/by-nd/4.0/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/1764252026-05-27T15:37:01Z
score 15.300719

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