Practical principles of density functional theory for catalytic reaction simulations on metal surfaces – from theory to applications

Abstract

In the past thirty years, molecular simulation techniques centred on density functional theory (DFT) calculations have quickly become a powerful research and technology development instrument. In particular, the knowledge and theory gained from DFT-based techniques have effectively transformed our understanding of the fundamental surface science, catalysis, and materials science. This review aims to provide a pedagogical narrative of the fundamentals of DFT and relevant computational methods applied for surface chemistry, catalytic reactions, particularly in the realm of heterogeneous and electrochemical catalysis. Several representative case studies in relation to energy and chemicals production are introduced, and relevant computationally driven catalyst design principles are discussed as well.

Keywords:

• Ammonia synthesis
• catalyst design
• computational catalysis
• density functional theory
• surface chemistry trends

Acknowledgements

N.S., M.Z. and B.L. thank the Start-up fund provided by Kansas State University, the National Science Foundation under Award No. EPS-0903806, and matching support from the State of Kansas through the Kansas Board of Regents for financial support. This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of DOE EPSCoR, under Award Number(s) DOE EPSCoR DE-FOA-0001572. J.C. and M.H. would like to thank the supports from National Science Foundation Grant: REU Site: Earth, Wind, and Fire: Sustainable Energy in the twenty-first Century; NSF Award No. 1460776. The authors are also grateful for the supercomputing resources and services from the Center for Nanoscale Materials (CNM) supported by the Office of Science of the US Department of Energy under the contract No. DE-AC02-06CH11357; the Beocat Research Cluster at Kansas State University, which is funded in part by NSF grants CNS-1006860; and the National Energy Research Scientific Computing Center (NERSC) under the contract No. DE-AC02-05CH11231.