Surface Reaction Barriometry: Methane Dissociation on Flat and Stepped Transition-Metal Surfaces

• DOI: 10.1021/acs.jpclett.7b01905
• Publication Date: 2017-08-17T21:17:29Z
• Authors: Davide Migliorini; Helen Chadwick; Francesco Nattino; Ana Gutiérrez-Gon...; Eric Dombrowski; Eric A. High; Han Guo; Arthur L. Utz; Bret Jackson; Rainer D. Beck; Geert-Jan Kroes
• Keywords: Transferability; Transition state theory

Accurately simulating heterogeneously catalyzed reactions requires reliable barriers for molecules reacting at defects on metal surfaces, such as steps. However, first-principles methods capable of computing these to chemical accuracy have yet be demonstrated. We show that state-resolved molecular beam experiments combined with ab initio dynamics using specific reaction parameter density functional theory (SRP-DFT) can determine the molecule-metal surface interaction required reliability. Crucially, SRP-DFT exhibits transferability: devised methane a flat (111) face Pt (and Ni) also describes its stepped Pt(211) accuracy. Our approach help bridge materials gap between fundamental science studies regular surfaces and heterogeneous catalysis in which defected are important.