相关论文: Cluster Catalysis with Lattice Oxygen: Tracing Oxy…
Metal-support interactions are frequently invoked to explain the enhanced catalytic activity of metal nanoparticles dispersed over reducible metal-oxide supports, yet the atomic scale mechanisms are rarely known. Here, we use scanning…
Heterogeneous catalysts based on sub-nanometer metal clusters often exhibit strongly size-dependent properties, and the addition or removal of a single atom can make all the difference. Identifying the most active species and deciphering…
Reducible oxides are widely used catalyst supports that can increase oxidation reaction rates by transferring their lattice oxygen at the metal-support interface. The interfacial oxidation process is typically described in terms of a…
A major challenge in electrochemistry is to decouple the reactive intermediates of a catalytic cycle to optimise their energies independently. During the oxygen evolution reaction (OER), such energy interdependence results from the need to…
Iron oxides play an increasingly prominent role in heterogeneous catalysis, hydrogen production, spintronics and drug delivery. The surface or material interface can be performance limiting in these applications, so it is vital to determine…
We present lattice-gas modeling of the steady-state behavior in CO oxidation on the facets of nanoscale metal clusters, with coupling via inter-facet CO diffusion. The model incorporates the key aspects of reaction process, such as rapid CO…
This work explores the role of oxygen in industrial methane oxidation. Oxygen, a well-known oxidizing agent, drives CH$_4$ conversion to CO$_2$ and H$_2$O. We report how oxygen influences oxidation on single Pd and PdO clusters supported on…
By applying a genetic algorithm in a cascade approach of increasing accuracy, we calculate the composition and structure of MgMOx clusters at realistic temperatures and oxygen pressures. The stable and metastable systems are identified by…
Metal-support interfaces fundamentally govern the catalytic performance of heterogeneous systems through complex interactions. Here, utilizing operando transmission electron microscopy, we uncovered a type of looping metal-support…
For large-scale deployment and use of polymer electrolyte fuel cells, high-performance electrocatalysts with low platinum consumption are desirable. One promising strategy to meet this demand is to explore alternative materials that retain…
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…
The (111) facet of magnetite (Fe$_3$O$_4$) has been studied extensively by experimental and theoretical methods, but controversy remains regarding the structure of its low-energy surface terminations. Using density functional theory (DFT)…
Oxygen exchange at oxide/liquid and oxide/gas interfaces is important in technology and environmental studies, as it is closely linked to both catalytic activity and material degradation. The atomic-scale details are mostly unknown,…
Recent DFT calculations for Ba2CoO4 (BCO) and neutron scattering experiments for SrRuO3 (SRO) have shown that oxygen develops a magnetic polarization. Moreover, DFT calculations for these compounds also unveiled unexpected nodes in the spin…
The coarsening of catalytically-active metal clusters is often accelerated by the presence of gases through the formation of mobile intermediates, though the exact mechanism through which this happens is often subject to debate. We use…
Catalysis is indispensable to chemical processes and relevant to many aspects of modern life. Owing to the intriguing electronic structures and good ionic properties, multivalent transition metal oxides have attracted attention as key…
We report on the structure and adsorption properties of Pd$_n$ ($n=1-4$) clusters supported on the rutile TiO$_2$ (110) surfaces with the possible presence of a surface oxygen vacancy or a subsurface Ti-interstitial atom. As predicted by…
Kinetic Monte-Carlo simulation is applied to study the partial oxidation of methane over a nickel catalyst. Based on the Langmuir-Hinshelwood mechanism, the kinetic behavior of this reaction is analyzed and the results are compared with…
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 investigate a driven diffusive lattice gas model with two oppositely moving species of particles. The model is motivated by bi-directional traffic of ants on a pre-existing trail. A third species, corresponding to pheromones used by the…