Related papers: A microscopic perspective on heterogeneous catalys…
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,…
Heterogenous reactions typically consist of multiple elementary steps and their rate coefficients are of fundamental importance in elucidating the mechanisms and micro-kinetics of these processes. Transition-state theory (TST) for…
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…
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…
We use multi-scale modeling to analyze laser-induced fluorescence (LIF) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density-functional theory based kinetic Monte Carlo simulations…
We investigate catalysis in the framework of elementary thermal operations, leveraging the distinct features of such operations to illuminate catalytic dynamics. As groundwork, we establish new technical tools that enhance the computability…
We present a density-functional theory based kinetic Monte Carlo study of CO oxidation at the (111) facet of RuO$_2$. We compare the detailed insight into elementary processes, steady-state surface coverages and catalytic activity to…
An external electric field (EEF) can impact a broad range of catalytic processes beyond redox systems. Computational design of catalysts under EEFs targeting specific operation conditions essentially requires accurate predictions of the…
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…
$\textit{In situ}$ environmental transmission electron microscopy (ETEM) is a powerful tool for observing structural modifications taking place in heterogeneous catalysts under reaction conditions. However, to strengthen the link between…
We study a model for unimolecular reaction on a supported catalyst including reactant diffusion and desorption, using analytical methods and scaling concepts. For rapid reactions, enhancing surface diffusion or increasing particle size…
Unique catalytic potential of metal surfaces has encouraged a great number of basic and applied studies. The manuscript highlights the general regularities in a field on the grounds of strong interrelation between catalytic, kinetic and…
Every mathematical model describing physical phenomena is an approximation to model reality, hence has its limitations. Depending on characteristic values of the variables in the model, different aspects of the model and, e.g.,…
A study by infrared spectroscopy of the physisorbed region of catalysis demonstrated that the intermediates of catalysis exist on the surface as a two dimensional gas. Data in the Atomic Energy Level tables show that of the thousands of…
The hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) play an important role in hydrogen based energy conversion. Recently, the frustrating performance in alkaline media raised debates on the relevant mechanism,…
Autonomous computations that rely on automated reaction network elucidation algorithms may pave the way to make computational catalysis on a par with experimental research in the field. Several advantages of this approach are key to…
Catalysis lies at the heart of chemical reactivity, yet its foundational principles remain fragmented across the distinct domains of homogeneous, heterogeneous, and enzymatic systems Here, we propose a unifying theoretical model that…
Heterogeneous catalysts are the most important catalysts in industrial reactions. Nanocatalysts, with size ranging from hundreds of nanometers to the atomic scale, possess activities that are closely connected to their structural…
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…
Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in…