Related papers: Evaluating continuum solvation models for the elec…
An important objective of designing lithium-ion rechargeable battery cells is to maximize their rate performance without compromising the energy density, which is mainly achieved through computationally expensive numerical simulations at…
The ab-initio computational treatment of electrochemical systems requires an appropriate treatment of the solid/liquid interfaces. A fully quantum mechanical treatment of the interface is computationally demanding due to the large number of…
Freestanding oxide films offer significant potential for integrating exotic quantum functionalities with semiconductor technologies. However, their performance is critically limited by surface roughness and interfacial imperfection caused…
Determining the solvation free energies of single ions in water is one of the most fundamental problems in physical chemistry and yet many unresolved questions remain. In particular, the ability to decompose the solvation free energy into…
The manner in which electrolyte solutions respond to electric fields is crucial to understanding the behavior of these systems both at, and away from, equilibrium. The present formulation of linear response theory for such systems is…
Using the example of a proton adsorption process, we analyze and compare two prominent modelling approaches in computational electrochemistry at metallic electrodes - electronically canonical, constant-charge and electronically…
In solid-state electrochemical experiments, the boundary between the sample and the electrolyte plays a crucial role, and the rest of the sample acting as a buffer that maintains a fixed composition. Due to the presence of an…
The underpotential deposition of transition metal ions is a critical step in many electrosynthetic approaches. While underpotential deposition has been intensively studied at the atomic level, first-principles calculations in vacuum can…
Electrochemical kinetics at electrode-electrolyte interfaces are crucial to understand high-rate behavior of energy storage devices. Phase transformation of electrodes is typically treated under equilibrium thermodynamic conditions, while…
Understanding the electrical double layer (EDL), i.e, the distribution of electrolyte at an electrified interface, in concentrated electrolytes is important for various technologies, such as supercapacitors, batteries and electrocatalysis.…
We introduce an adhesion parameter that enables rapid screening for materials interfaces with high adhesion. This parameter is obtained by density functional theory calculations of individual single-material slabs rather than slabs…
Continuum solvation models enable efficient first principles calculations of chemical reactions in solution, but require extensive parametrization and fitting for each solvent and class of solute systems. Here, we examine the assumptions of…
We studied polyelectrolyte adsorption on a repulsive charged surface by scaling analysis. At low ionic strength and low surface charge density in which a single polyelectrolyte is able to be adsorbed onto the surface, different regimes in…
The problem of the equilibrium state of the charged many-particle system above dielectric surface is formulated.We consider the case of the presence of the external attractive pressing field and the case of its absence. The equilibrium…
We study, using Density Functional theory and Monte Carlo simulations, aqueous electrolyte solutions between charged infinite planar surfaces, in a contact with a bulk salt reservoir. In agreement with recent experimental observations [Z.…
While fluids near a solid surface are at the core of applications in energy storage/conversion, electrochemistry/electrowetting and adsorption/catalysis, their nanoscale behavior remains only partially deciphered. Beyond conventional…
Highly accurate methods such as coupled cluster (CC) techniques can be used for periodic systems within the framework of the method of increments. Its extension to low-dimensional conducting system is considered. To demonstrate the…
We review a model for a solid electrolyte derived under thermodynamics principles. We non-dimensionalise and scale the model to identify small parameters, where we identify a scaling that controls the width of the space-charge layer in the…
The interaction between charged objects in solution is generally expected to recapitulate two central principles of electromagnetics: (i) like-charged objects repel, and (ii) they do so regardless of the sign of their electrical charge.…
Rechargeable battery electrodes have highly complex microstructures, consisting of nonuniform electrode particles, tortuous electrolyte channels, and irregular particle-electrolyte interfaces. Moreover, the electrochemical processes involve…