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Title: Structure of the Electric Double Layer in Hydrothermal Systems. Molecular Simulation Approach and Interpretation of Experimental Results

Abstract

When an aqueous electrolyte solution is put in contact with a solid surface the solid-liquid interface develops a net electric polarization resulting from the formation of an electric double layer. While this phenomenon has been known for more than a century, giving rise to a variety of theories including the first one by Helmholtz followed by Gouy-Chapman (Israelachvili 1992), and Bockris-Devanathan-Miller (Bockris, Devanathan et al. 1963). The existence of the electric double layer has a strong impact on many chemical (electrochemical metal deposition, corrosion, catalysis), biochemical (ion channels), and geological (mineral dissolution/deposition and reactivity, crystallization) processes due to charge-shielding resulting from the movement of ions toward the interface to balance the charged surface. Typically, the theoretical investigation of the microscopic structure of the medium near the (charged or uncharged) interface has been done with simplified models, involving a structure less surface in contact with point (or hard-sphere) ions immersed in a dielectric continuum (Schmickler and Henderson 1986). Obviously, these models neglect important physicochemical aspects of the system, such as the solvent structure around the species in solution (solvation effects), as well as the reactive interaction between the solvent and the solid surface. In order to interpret the actual electrochemical behaviormore » of ionic species in solution, their interaction with the solid surface and their mobility we need to develop molecular-based tools. These tools must take explicitly into account the discrete nature of all species in solution and the essential features to describe the solid surface and its interactions with the contact solution (ultimately, it will include the discrete nature of the surface). The main goal of our research is the analysis of the microscopic behavior of high-temperature aqueous electrolyte solutions in contact with metal oxide surfaces, to gain an improve d understanding of the configurational behavior of the electric double layer. For that purpose we develop molecular dynamics protocols to characterize formation of the electric double layer through the determination of the profiles of species' concentrations, electric field, species diffusivity, and solvent polarization normal to the oxide surface.« less

Authors:
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
US Department of Energy (US)
OSTI Identifier:
787479
Report Number(s):
P01-111111
TRN: US200203%%113
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Conference
Resource Relation:
Conference: Annual Meeting of the AICHE, Reno, USA (US), 11/04/2001; Other Information: PBD: 19 Jun 2001
Country of Publication:
United States
Language:
English
Subject:
15 GEOTHERMAL ENERGY; 36 MATERIALS SCIENCE; CATALYSIS; CORROSION; CRYSTALLIZATION; DEPOSITION; DIELECTRIC MATERIALS; ELECTRIC FIELDS; ELECTROLYTES; HYDROTHERMAL SYSTEMS; OXIDES; POLARIZATION; SOLVENTS; Geothermal Legacy

Citation Formats

Chialvo, A A. Structure of the Electric Double Layer in Hydrothermal Systems. Molecular Simulation Approach and Interpretation of Experimental Results. United States: N. p., 2001. Web.
Chialvo, A A. Structure of the Electric Double Layer in Hydrothermal Systems. Molecular Simulation Approach and Interpretation of Experimental Results. United States.
Chialvo, A A. 2001. "Structure of the Electric Double Layer in Hydrothermal Systems. Molecular Simulation Approach and Interpretation of Experimental Results". United States. https://www.osti.gov/servlets/purl/787479.
@article{osti_787479,
title = {Structure of the Electric Double Layer in Hydrothermal Systems. Molecular Simulation Approach and Interpretation of Experimental Results},
author = {Chialvo, A A},
abstractNote = {When an aqueous electrolyte solution is put in contact with a solid surface the solid-liquid interface develops a net electric polarization resulting from the formation of an electric double layer. While this phenomenon has been known for more than a century, giving rise to a variety of theories including the first one by Helmholtz followed by Gouy-Chapman (Israelachvili 1992), and Bockris-Devanathan-Miller (Bockris, Devanathan et al. 1963). The existence of the electric double layer has a strong impact on many chemical (electrochemical metal deposition, corrosion, catalysis), biochemical (ion channels), and geological (mineral dissolution/deposition and reactivity, crystallization) processes due to charge-shielding resulting from the movement of ions toward the interface to balance the charged surface. Typically, the theoretical investigation of the microscopic structure of the medium near the (charged or uncharged) interface has been done with simplified models, involving a structure less surface in contact with point (or hard-sphere) ions immersed in a dielectric continuum (Schmickler and Henderson 1986). Obviously, these models neglect important physicochemical aspects of the system, such as the solvent structure around the species in solution (solvation effects), as well as the reactive interaction between the solvent and the solid surface. In order to interpret the actual electrochemical behavior of ionic species in solution, their interaction with the solid surface and their mobility we need to develop molecular-based tools. These tools must take explicitly into account the discrete nature of all species in solution and the essential features to describe the solid surface and its interactions with the contact solution (ultimately, it will include the discrete nature of the surface). The main goal of our research is the analysis of the microscopic behavior of high-temperature aqueous electrolyte solutions in contact with metal oxide surfaces, to gain an improve d understanding of the configurational behavior of the electric double layer. For that purpose we develop molecular dynamics protocols to characterize formation of the electric double layer through the determination of the profiles of species' concentrations, electric field, species diffusivity, and solvent polarization normal to the oxide surface.},
doi = {},
url = {https://www.osti.gov/biblio/787479}, journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Jun 19 00:00:00 EDT 2001},
month = {Tue Jun 19 00:00:00 EDT 2001}
}

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