Related papers: Structure Sensitivity in Oxide Catalysis: First-Pr…
We describe a first-principles statistical mechanics approach enabling us to simulate the steady-state situation of heterogeneous catalysis. In a first step density-functional theory together with transition-state theory is employed to…
Using the catalytic CO oxidation at RuO2(110) as a showcase, we employ first-principles kinetic Monte Carlo simulations to illustrate the intricate effects on temperature programmed reaction spectroscopy data brought about by the mere…
In recent years due to improvements in calculation methods and increased computer power, it has become possible to perform first-principles investigations for ``simple'' chemical reactions at surfaces. We have carried out such studies for…
Lattice kinetic Monte Carlo simulations have become a vital tool for predictive quality atomistic understanding of complex surface chemical reaction kinetics over a wide range of reaction conditions. In order to expand their practical value…
We present a first-principles based multiscale modeling approach to heterogeneous catalysis that integrates first-principles kinetic Monte Carlo simulations of the surface reaction chemistry into a fluid dynamical treatment of the…
The phase diagram of surface structures for the model catalyst RuO2(110) in contact with a gas environment of O2 and CO is calculated by density-functional theory and atomistic thermodynamics. Adsorption of the reactants is found to depend…
The possible importance of oxide formation for the catalytic activity of transition metals in heterogenous oxidation catalysis has evoked a lively discussion over the recent years. On the more noble transition metals (like Pd, Pt or Ag) the…
We present a multi-lattice kinetic Monte Carlo (kMC) approach that efficiently describes the atomistic dynamics of morphological transitions between commensurate structures at crystal surfaces. As an example we study the reduction of a…
We present first-principles kinetic Monte Carlo (1p-kMC) simulations addressing the CO oxidation reaction at Pd(100) for gas-phase conditions ranging from ultra-high vacuum (UHV) to ambient pressures and elevated temperatures. For the…
The turn-over frequency of the catalytic oxidation of CO at RuO2(110) was calculated as function of temperature and partial pressures using ab initio statistical mechanics. The underlying energetics of the gas-phase molecules, dissociation,…
Recent experiments revealed an anomalous dependence of carbon monoxide oxidation at Ru(0001) on oxygen pressure and a particularly high reaction rate. Below we report density functional theory calculations of the energetics and reaction…
Knowledge of the atomic geometry of a surface is a prerequisite for any detailed understanding of the surface's electronic structure and chemical properties. Previous studies have convincingly demonstrated that density functional theory…
Using density functional theory and an exchange-correlationfunctional that includes the van der Waals interaction, we study the coadsorption of CO on Ru(0001) saturated with 0.5 ML of oxygen. Different coexisting CO coverages are considered…
Experiments performed at high gas partial pressures have demonstrated that the kinetics of the CO oxidation reaction at Ru(0001) is different and somewhat anomalous compared to that over other transition metal surfaces and, in particular,…
We present a density-functional theory based Wulff construction of the equilibrium shape of RuO2 particles in an oxygen environment. The obtained intricate variations of the crystal habit with the oxygen chemical potential allow for a…
We employ a multiscale modeling approach to study the surface structure and composition of a Pd(100) model catalyst in reactive environments. Under gas phase conditions representative of technological CO oxidation (~1 atm, 300-600 K) we…
The possible formation of oxides or thin oxide films (surface oxides) on late transition metal surfaces is recently being recognized as an essential ingredient when aiming to understand catalytic oxidation reactions under technologically…
Understanding the atomic mechanism of low-temperature CO oxidation on a heterogeneous catalyst is challenging. We performed density functional theory (DFT) calculations to identify the surface structure and reaction mechanism responsible…
Using density-functional theory (DFT) we calculate the Gibbs free energy to determine the lowest-energy structure of a RuO_2(110) surface in thermodynamic equilibrium with an oxygen-rich environment. The traditionally assumed stoichiometric…
Density functional theory (DFT) is widely used in surface science, but gives poor accuracy for oxide surface processes, while high-level quantum chemistry methods are hard to apply without losing basis-set quality. We argue that quantum…