Understanding interfacial structure and preferential adsorption in mixed alkali-halide electrolytes at graphene oxide electrodes by constant potential molecular dynamics simulations

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F67985858%3A_____%2F25%3A00616476" target="_blank" >RIV/67985858:_____/25:00616476 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/60076658:12310/25:43911224

Výsledek na webu

<a href="https://www.sciencedirect.com/science/article/pii/S0167732225002375?via%3Dihub" target="_blank" >https://www.sciencedirect.com/science/article/pii/S0167732225002375?via%3Dihub</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.molliq.2025.127078" target="_blank" >10.1016/j.molliq.2025.127078</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Understanding interfacial structure and preferential adsorption in mixed alkali-halide electrolytes at graphene oxide electrodes by constant potential molecular dynamics simulations

Popis výsledku v původním jazyce

Graphene oxide (GO) is a promising material that finds use in electrochemical applications. Therefore, understanding the microscopic behavior of electrolytes in contact with GO electrodes is important. In this work, we focus on a detailed description and explanation of the structure, adsorption behavior, and self-diffusion of aqueous solutions of single-salt and mixed-cation alkali metal chlorides in the vicinity of hydroxylated GO electrodes under normal thermodynamic conditions and varying interelectrode voltages. We performed molecular dynamics simulations of the solutions constrained between planar GO electrodes using the constant potential method. We analyzed several structural properties, including prfiles of atomic density, charge density,ncharacteristics of the network of non-covalent bonds, and in-plane and transverse self-diffusion, all as functions of the distance from the GO surface. We discuss and explain the behavior of all these properties in detail as a result of three driving forces: (i) the direct electrode-solution interactions, (ii) the tendency of the solutions to saturate the network of non-covalent bonds, and (iii) the tendency of the system to suppress local charge accumulationnin any region larger than typical interparticle distances. The existence of hydroxyl groups here greatly enhances the direct electrode-solution interactions, causing qualitative differences in the structure, including a different arrangement of the adsorption layers of ions in comparison to the solutions at graphene electrodes.

Název v anglickém jazyce

Understanding interfacial structure and preferential adsorption in mixed alkali-halide electrolytes at graphene oxide electrodes by constant potential molecular dynamics simulations

Popis výsledku anglicky

Graphene oxide (GO) is a promising material that finds use in electrochemical applications. Therefore, understanding the microscopic behavior of electrolytes in contact with GO electrodes is important. In this work, we focus on a detailed description and explanation of the structure, adsorption behavior, and self-diffusion of aqueous solutions of single-salt and mixed-cation alkali metal chlorides in the vicinity of hydroxylated GO electrodes under normal thermodynamic conditions and varying interelectrode voltages. We performed molecular dynamics simulations of the solutions constrained between planar GO electrodes using the constant potential method. We analyzed several structural properties, including prfiles of atomic density, charge density,ncharacteristics of the network of non-covalent bonds, and in-plane and transverse self-diffusion, all as functions of the distance from the GO surface. We discuss and explain the behavior of all these properties in detail as a result of three driving forces: (i) the direct electrode-solution interactions, (ii) the tendency of the solutions to saturate the network of non-covalent bonds, and (iii) the tendency of the system to suppress local charge accumulationnin any region larger than typical interparticle distances. The existence of hydroxyl groups here greatly enhances the direct electrode-solution interactions, causing qualitative differences in the structure, including a different arrangement of the adsorption layers of ions in comparison to the solutions at graphene electrodes.

Druh

J_SC - Článek v periodiku v databázi SCOPUS

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GA21-27338S" target="_blank" >GA21-27338S: Kapacitní deionizace: Porozumění pomocí molekulárního modelování</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Molecular Liquids

ISSN

0167-7322

e-ISSN

1873-3166

Svazek periodika

424

Číslo periodika v rámci svazku

15 April

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

14

Strana od-do

127078

Kód UT WoS článku

—

EID výsledku v databázi Scopus

2-s2.0-85216895946