High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials

Molecular simulations provide a versatile tool to study the structure, anion conductivity, and stability of anion-exchange membrane (AEM) materials and can provide a fundamental understanding of the relation between structure and property of membranes that is key for their use in fuel cells and othe...

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Autores principales:	Lu, J., Jacobson, L.C., Perez Sirkin, Y.A., Molinero, V.
Formato:	JOUR
Acceso en línea:	http://hdl.handle.net/20.500.12110/paper_15499618_v13_n1_p245_Lu
Aporte de:	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires

id	todo:paper_15499618_v13_n1_p245_Lu
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spelling	todo:paper_15499618_v13_n1_p245_Lu2023-10-03T16:23:17Z High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials Lu, J. Jacobson, L.C. Perez Sirkin, Y.A. Molinero, V. Molecular simulations provide a versatile tool to study the structure, anion conductivity, and stability of anion-exchange membrane (AEM) materials and can provide a fundamental understanding of the relation between structure and property of membranes that is key for their use in fuel cells and other applications. The quest for large spatial and temporal scales required to model the multiscale structure and transport processes in the polymer electrolyte membranes, however, cannot be met with fully atomistic models, and the available coarse-grained (CG) models suffer from several challenges associated with their low-resolution. Here, we develop a high-resolution CG force field for hydrated polyphenylene oxide/trimethylamine chloride (PPO/TMACl) membranes compatible with the mW water model using a hierarchical parametrization approach based on Uncertainty Quantification and reference atomistic simulations modeled with the Generalized Amber Force Field (GAFF) and TIP4P/2005 water. The parametrization weighs multiple properties, including coordination numbers, radial distribution functions (RDFs), self-diffusion coefficients of water and ions, relative vapor pressure of water in the solution, hydration enthalpy of the tetramethylammonium chloride (TMACl) salt, and cohesive energy of its aqueous solutions. We analyze the interdependence between properties and address how to compromise between the accuracies of the properties to achieve an overall best representability. Our optimized CG model FFcomp quantitatively reproduces the diffusivities and RDFs of the reference atomistic model and qualitatively reproduces the experimental relative vapor pressure of water in solutions of tetramethylammonium chloride. These properties are of utmost relevance for the design and operation of fuel cell membranes. To our knowledge, this is the first CG model that includes explicitly each water and ion and accounts for hydrophobic, ionic, and intramolecular interactions explicitly parametrized to reproduce multiple properties of interest for hydrated polyelectrolyte membranes. The CG model of hydrated PPO/TMACl water is about 100 times faster than the reference atomistic GAFF-TIP4P/2005 model. The strategy implemented here can be used in the parametrization of CG models for other substances, such as biomolecular systems and membranes for desalination, water purification, and redox flow batteries. We anticipate that the large spatial and temporal simulations made possible by the CG model will advance the quest for anion-exchange membranes with improved transport and mechanical properties. © 2016 American Chemical Society. Fil:Molinero, V. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_15499618_v13_n1_p245_Lu
institution	Universidad de Buenos Aires
institution_str	I-28
repository_str	R-134
collection	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
description	Molecular simulations provide a versatile tool to study the structure, anion conductivity, and stability of anion-exchange membrane (AEM) materials and can provide a fundamental understanding of the relation between structure and property of membranes that is key for their use in fuel cells and other applications. The quest for large spatial and temporal scales required to model the multiscale structure and transport processes in the polymer electrolyte membranes, however, cannot be met with fully atomistic models, and the available coarse-grained (CG) models suffer from several challenges associated with their low-resolution. Here, we develop a high-resolution CG force field for hydrated polyphenylene oxide/trimethylamine chloride (PPO/TMACl) membranes compatible with the mW water model using a hierarchical parametrization approach based on Uncertainty Quantification and reference atomistic simulations modeled with the Generalized Amber Force Field (GAFF) and TIP4P/2005 water. The parametrization weighs multiple properties, including coordination numbers, radial distribution functions (RDFs), self-diffusion coefficients of water and ions, relative vapor pressure of water in the solution, hydration enthalpy of the tetramethylammonium chloride (TMACl) salt, and cohesive energy of its aqueous solutions. We analyze the interdependence between properties and address how to compromise between the accuracies of the properties to achieve an overall best representability. Our optimized CG model FFcomp quantitatively reproduces the diffusivities and RDFs of the reference atomistic model and qualitatively reproduces the experimental relative vapor pressure of water in solutions of tetramethylammonium chloride. These properties are of utmost relevance for the design and operation of fuel cell membranes. To our knowledge, this is the first CG model that includes explicitly each water and ion and accounts for hydrophobic, ionic, and intramolecular interactions explicitly parametrized to reproduce multiple properties of interest for hydrated polyelectrolyte membranes. The CG model of hydrated PPO/TMACl water is about 100 times faster than the reference atomistic GAFF-TIP4P/2005 model. The strategy implemented here can be used in the parametrization of CG models for other substances, such as biomolecular systems and membranes for desalination, water purification, and redox flow batteries. We anticipate that the large spatial and temporal simulations made possible by the CG model will advance the quest for anion-exchange membranes with improved transport and mechanical properties. © 2016 American Chemical Society.
format	JOUR
author	Lu, J. Jacobson, L.C. Perez Sirkin, Y.A. Molinero, V.
spellingShingle	Lu, J. Jacobson, L.C. Perez Sirkin, Y.A. Molinero, V. High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials
author_facet	Lu, J. Jacobson, L.C. Perez Sirkin, Y.A. Molinero, V.
author_sort	Lu, J.
title	High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials
title_short	High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials
title_full	High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials
title_fullStr	High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials
title_full_unstemmed	High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials
title_sort	high-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials
url	http://hdl.handle.net/20.500.12110/paper_15499618_v13_n1_p245_Lu
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High-resolution coarse-grained model of hydrated anion-exchange membranes that accounts for hydrophobic and ionic interactions through short-ranged potentials

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