First-principles, atomistic thermodynamics for oxidation catalysis

TL;DR

This paper develops a method using ab initio atomistic thermodynamics to create phase diagrams of surface structures across a wide range of temperatures and pressures, enhancing understanding of catalytic processes under realistic conditions.

Contribution

It introduces a comprehensive approach to predict surface phases at operational conditions, bridging the gap between low-pressure studies and real-world catalytic environments.

Findings

Phase diagrams spanning ultra-high vacuum to industrial conditions

Identification of stable surface structures at various T,p conditions

Highlighting the importance of reaction kinetics near phase boundaries

Abstract

Present knowledge of the function of materials is largely based on studies (experimental and theoretical) that are performed at low temperatures and ultra-low pressures. However, the majority of everyday applications, like e.g. catalysis, operate at atmospheric pressures and temperatures at or higher than 300 K. Here we employ ab initio, atomistic thermodynamics to construct a phase diagram of surface structures in the (T,p)-space from ultra-high vacuum to technically-relevant pressures and temperatures. We emphasize the value of such phase diagrams as well as the importance of the reaction kinetics that may be crucial e.g. close to phase boundaries.