相关论文: Revisiting the Electrified Pt(111)/Water Interface…
While first-principles calculations of electrode-molecule binding play an indispensable role in obtaining atomic-level understanding in surface science and electrochemistry, a significant challenge remains because the adsorption energy is…
Electrical double layers play a key role in a variety of electrochemical systems. The mean free path of secondary electrons in aqueous solutions is on the order of a nanometer, making them suitable for probing of ultrathin electrical double…
The interface between liquid water and the Pt(111) metal surface is characterized structurally and thermodynamically via reactive molecular dynamics (MD) simulations within the ReaxFF framework. The formation of a distinct buckled adsorbate…
The ab initio simulation of charged interfaces in the framework of density functional theory (DFT) is heavily employed for the study of electrochemical energy conversion processes. The capacitance is the primary descriptor for the response…
The design of better heterogeneous catalysts for applications such as fuel cells and electrolyzers requires a mechanistic understanding of electrocatalytic reactions and the dependence of their activity on operating conditions such as pH. A…
The open water surface is known to be charged. Yet, the magnitude of the charge and the physical mechanism of the charging remain unclear, causing heated debates across the scientific community. Here we directly measure the charge Q of…
Quantum-chemical processes in liquid environments impact broad areas of science, from molecular biology to geology to electrochemistry. While density-functional theory (DFT) has enabled efficient quantum-mechanical calculations which…
Orbital-free density functional theory (OF-DFT) provides an alternative approach for calculating the molecular electronic energy, relying solely on the electron density. In OF-DFT, both the ground-state density is optimized variationally to…
This work explores the use of joint density-functional theory, a new form of density-functional theory for the ab initio description of electronic systems in thermodynamic equilibrium with a liquid environment, to describe electrochemical…
A simplified density functional theory (DFT) method for charged adsorbates on an ultrathin, insulating film supported by a metal substrate is developed and presented. This new method is based on a previous DFT development that uses a…
We analyze and compare the structural, dynamical, and electronic properties of liquid water next to prototypical metals including Pt, graphite, and graphene. Our results are built on Born-Oppenheimer molecular dynamics (BOMD) generated…
Platinum-water interfaces underpin many electrochemical energy conversion processes. However, despite decades of research, the real-space liquid structure of these interfaces remains elusive. Using three-dimensional atomic force microscopy…
The potential of zero free charge (PZFC) value is a crucial parameter in electrochemistry. However, the evaluations of PZFC have traditionally been difficult. To overcome this challenge, we applied a hybrid solvation method that…
Atomistic simulations of electrochemical interfaces remain challenging due to the long time scales required to adequately sample the structure of the electric double layer. The emergence of efficient, short-range machine learning…
A general set of methods is presented for calculating chemical potentials in solid and liquid mixtures using {\em ab initio} techniques based on density functional theory (DFT). The methods are designed to give an {\em ab initio} approach…
Understanding strongly correlated systems is essential for advancing quantum chemistry and materials science, yet conventional methods like Density Functional Theory (DFT) often fail to capture their complex electronic behavior. To address…
Classical density-functional theory provides an efficient alternative to molecular dynamics simulations for understanding the equilibrium properties of inhomogeneous fluids. However, application of density-functional theory to multi-site…
The ongoing scientific interest in the properties and structure of electric double layers (EDLs) stems from their pivotal role in (super)capacitive energy storage, energy harvesting, and water treatment technologies. Classical density…
This work assesses a classical density functional theory (DFT) model for predicting macroscopic static contact angles of pure substances and mixtures by comparison to own experimental data. We employ a DFT with a Helmholtz energy functional…
Computational studies of electrochemical interfaces based on density-functional theory (DFT) play an increasingly important role in present research on electrochemical processes for energy conversion and storage. The homogeneous background…