Related papers: Water-Induced Bimetallic Alloy Surface Segregation…
We use density functional theory (DFT) with the generalized gradient approximation (GGA) and our first-principles extrapolation method for accurate chemisorption energies {[Mason {\em et al.}, Phys. Rev. B {\bf 69}, 161401R (2004)]} to…
Recent measurements show that the free surfaces of liquid metals and alloys are always layered, regardless of composition and surface tension; a result supported by three decades of simulations and theory. Recent theoretical work claims,…
We studied the surface properties of Ga-Cu based liquid metal alloys, a promising material system for supported catalytically active liquid metal solutions (SCALMS). The impact of Cu dilution in the (liquid) Ga matrix is in-detail…
The structure of a water adlayer on Pt(111) surface is investigated by extensive first principle calculations. Only allowing for proton disorder the ground state energy can be found. This results from an interplay between water/metal…
Using a new form of density functional theory for the {\em ab initio} description of electronic systems in contact with a dielectric environment, we present the first detailed study of the impact of a solvent on the surface chemistry of…
Molecular dynamics simulations combined with periodic electronic structure calculations are performed to decipher structural, thermodynamical and dynamical properties of the interfaced vs. confined water adsorbed in hexagonal 1D channels of…
Multi-component alloys offer broad tunability for addressing challenges in materials science, but their vast configurational space makes their surface chemistry highly sensitive to operating conditions, for example through adsorption and…
We report the effect of interstitial fluid on the extent of segregation by imaging the pile that results after bidisperse color-coded particles are poured into a silo. Segregation is sharply reduced and preferential clumping of small…
The interaction of water with $\alpha$-alumina (i.e. $\alpha$-Al$_{2}$O$_{3}$ surfaces is important in a variety of applications and a useful model for the interaction of water with environmentally abundant aluminosilicate phases. Despite…
First-principles calculations are a cornerstone of modern surface science and heterogeneous catalysis. However, accurate reaction energies and barrier heights are frequently inaccessible due to the approximations demanded by the large…
Copper-based catalysts are of particular interest for electrochemical reduction of CO$_2$ (CO2RR) as products beyond CO can form. To improve activity and selectivity, several studies have focused on the addition of other elements as…
We present a first-principles atomistic thermodynamics framework to describe the structure, composition and segregation profile of an alloy surface in contact with a (reactive) environment. The method is illustrated with the application to…
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…
Alkali metals are known as efficient promoters in heterogeneous catalysis but the nature of this phenomenon is as yet not understood. Our first principles calculations reveal a huge increase and delocalization of the isoelectronic…
The key kinetic barrier to dolomite formation is related to the surface Mg2+-H2O complex, which hinders binding of surface Mg2+ ions to the CO3 2- ions in solution. It has been proposed that this reaction can be catalyzed by dissolved…
The interaction of water with Fe$_3$O$_4$(001) is studied by density functional theory (DFT) calculations including an on-site Coulomb term. For isolated molecules dissociative adsorption is strongly promoted at surface defect sites, while…
Segregation of alloying elements and impurities at grain boundaries (GBs) critically influences material behavior by affecting cohesion. In this study, we present an ab initio high-throughput evaluation of segregation energies and cohesive…
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 interaction of water with oxide surfaces is of great interest for both fundamental science and applications. We present a combined theoretical [density functional theory (DFT)] and experimental [Scanning Tunneling Microscopy (STM),…
Water dissociation is of fundamental importance in scientific fields and has drawn considerable interest in diverse technological applications. However, the high activation barrier of breaking the O-H bond within the water molecule has been…