Multi-scale simulation of the adsorption of lithium ion on graphite surface: From quantum Monte Carlo to molecular density functional theory

Ruggeri, Michele; Reeves, Kyle; Hsu, Tzu-Yao; Jeanmairet, Guillaume; Salanne, Mathieu; Pierleoni, Carlo

doi:10.1063/5.0082944

“…Carbon materials have been extensively studied, with idealized structures such as pristine carbon walls and carbon nanotubes (CNTs) − as well as complex porous structures. − It has been observed that liquids in confinement and at interfaces behave significantly different than in bulk. For example, changes in the packing and the rearrangement dynamics within the liquid can be observed. ,,− …”

Section: Introductionmentioning

confidence: 99%

CONAN─Novel Tool to Create and Analyze Liquids in Confined Space

Dick,

Kirchner

2023

J. Chem. Inf. Model.

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Modeling of complex liquids at solid surfaces and in confinement is gaining attention due to an increase in computer power and advancement of simulation techniques. Therefore, tools to set up structures and for analysis are needed. In this paper, we present CONANa Python code designed to facilitate the study of liquids interacting with solid structures, such as walls or pores. Among other things, the program provides the option to generate a variety of different structures, including carbon walls and nanotubes and their boron nitride analogs, as well as the ability to analyze various structural properties of confined and interfacial liquids. In the case of the ionic liquid 1-butyl-3-methylimidazolium acetate in carbon nanotubes of different sizes, we demonstrate the abilities of our tool. The average density within the confinement highly depends on the carbon nanotube size, and it is generally lower than the density of the bulk liquid. The arrangement of the individual species within the tube also depends on size, with radial layers forming within the tubular confinement. The density is largely increased in the respective layers, while it is drastically reduced between the layers.

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“…Approaches based on high-level ab initio calculations will certainly provide an important input towards this direction. 78,79…”

Section: Discussionmentioning

confidence: 99%

MetalWalls: Simulating electrochemical interfaces between polarizable electrolytes and metallic electrodes

Coretti

¹

,

Bacon

²

,

Berthin

³

et al. 2022

The Journal of Chemical Physics

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Electrochemistry is central to many applications, ranging from biology to energy science. Studies now involve a wide range of techniques, both experimental and theoretical. Modelling and simulations methods, such as density functional theory or molecular dynamics, provide key information on the structural and dynamic properties of the systems. Of particular importance are polarization effects the electrode/electrolyte interface, which are difficult to simulate accurately. Here we show how these electrostatic interactions are taken into account in the framework of the Ewald summation method. We discuss, in particular, the formal set up for calculations that enforce periodic boundary conditions in two directions, a geometry that more closely reflects the characteristics of typical electrolyte/electrode systems and presents some differences with respect to the more common case of periodic boundary conditions in three dimensions. These formal developments are implemented and tested in MetalWalls, a molecular dynamics software which captures the polarization of the electrolyte and allows the simulation of electrodes maintained at a constant potential. We also discuss the technical aspects involved in the calculation of two sets of coupled degrees of freedom, namely the induced dipoles and the electrode charges. We validate the implementation, first on simple systems, then on the well-known interface between graphite electrodes and a room-temperature ionic liquid. We finally illustrate the capabilities of MetalWalls by studying the adsorption of a complex functionalized electrolyte on a graphite electrode.

show abstract

“…Approaches based on high-level ab initio calculations will certainly provide an important input towards this direction. 76,77…”

Section: Discussionmentioning

confidence: 99%

MetalWalls: Simulating electrochemical interfaces between polarizable electrolytes and metallic electrodes

Coretti

¹

,

Bacon

²

,

Berthin

³

et al. 2022

Preprint

Self Cite

View full text Add to dashboard Cite

Electrochemistry is central to many applications, ranging from biology to energy science. Studies now involve a wide range of techniques, both experimental and theoretical. Modelling and simulations methods, such as density functional theory or molecular dynamics, provide key information on the structural and dynamic properties of the systems. Of particular importance are polarization effects the electrode/electrolyte interface, which are difficult to simulate accurately. Here we show how these electrostatic interactions are taken into account in the framework of the Ewald summation method. We discuss, in particular, the formal set up for calculations that enforce periodic boundary conditions in two directions, a geometry that more closely reflects the characteristics of typical electrolyte/electrode systems and presents some differences with respect to the more common case of periodic boundary conditions in three dimensions. These formal developments are implemented and tested in MetalWalls, a molecular dynamics software which captures the polarization of the electrolyte and allows the simulation of electrodes maintained at a constant potential. We also discuss the technical aspects involved in the calculation of two sets of coupled degrees of freedom, namely the induced dipoles and the electrode charges. We validate the implementation, first on simple systems, then on the well-known interface between graphite electrodes and a room-temperature ionic liquid. We finally illustrate the capabilities of MetalWalls by studying the adsorption of a complex functionalized electrolyte on a graphite electrode.

show abstract

Multi-scale simulation of the adsorption of lithium ion on graphite surface: From quantum Monte Carlo to molecular density functional theory

Cited by 9 publications

References 52 publications

CONAN─Novel Tool to Create and Analyze Liquids in Confined Space

CONAN─Novel Tool to Create and Analyze Liquids in Confined Space

MetalWalls: Simulating electrochemical interfaces between polarizable electrolytes and metallic electrodes

MetalWalls: Simulating electrochemical interfaces between polarizable electrolytes and metallic electrodes

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