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First-Principles Atomistic Thermodynamics for Oxidation Catalysis: Surface Phase Diagrams and Catalytically Interesting Regions

2002/11/26 by Karsten Reuter, Matthias Scheffler · 462 citations
Chemical Engineering · Chemistry · Materials Science · Physics and Astronomy · #Ab initio #Advanced Chemical Physics Studies #Catalysis and Oxidation Reactions #Catalytic Processes in Materials Science #Chemical physics #Chemistry #Kinetics #Materials science #Organic chemistry #Phase (matter) #Phase diagram #Physical chemistry #Physics #Quantum mechanics #Surface (topology) #Thermodynamics #cond-mat.mtrl-sci

paper · pdf · doi:10.1103/physrevlett.90.046103

published in Physical Review Letters 90(4), 046103 (American Physical Society) · 4 pages including 2 figure files. Submitted to Phys. Rev. Lett. Related publications can be found at http://www.fhi-berlin.mpg.de/th/paper.html

arxiv created 2002/11/26 · openalex publication_date 2003/01/30 · arxiv updated 2009/11/30 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05

Abstract

Present knowledge of the function of materials is largely based on studies (experimental and theoretical) that are performed at low temperatures and ultralow 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 ultrahigh 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.

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