title: Catalysis. Assessing the reliability of calculated catalytic ammonia synthesis rates.
abstract: We introduce a general method for estimating the uncertainty in calculated materials properties based on density functional theory calculations. We illustrate the approach for a calculation of the catalytic rate of ammonia synthesis over a range of transition-metal catalysts. The correlation between errors in density functional theory calculations is shown to play an important role in reducing the predicted error on calculated rates. Uncertainties depend strongly on reaction conditions and catalyst material, and the relative rates between different catalysts are considerably better described than the absolute rates. We introduce an approach for incorporating uncertainty when searching for improved catalysts by evaluating the probability that a given catalyst is better than a known standard.
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 94305, USA.
authors.forename: Andrew J
authors.initials: AJ
authors.lastname: Medford
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 94305, USA.
authors.forename: Jess
authors.initials: J
authors.lastname: Wellendorff
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: Aleksandra
authors.initials: A
authors.lastname: Vojvodic
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: Felix
authors.initials: F
authors.lastname: Studt
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: Frank
authors.initials: F
authors.lastname: Abild-Pedersen
authors.affiliation: Center for Atomic-scale Materials Design (CAMD), Department of Physics, Technical University of Denmark, DK-2800 Lyngby, Denmark.
authors.forename: Karsten W
authors.initials: KW
authors.lastname: Jacobsen
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: Thomas
authors.initials: T
authors.lastname: Bligaard
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 94305, USA. norskov@stanford.edu.
authors.forename: Jens K
authors.initials: JK
authors.lastname: Nørskov