title: Finding optimal surface sites on heterogeneous catalysts by counting nearest neighbors.
abstract: A good heterogeneous catalyst for a given chemical reaction very often has only one specific type of surface site that is catalytically active. Widespread methodologies such as Sabatier-type activity plots determine optimal adsorption energies to maximize catalytic activity, but these are difficult to use as guidelines to devise new catalysts. We introduce "coordination-activity plots" that predict the geometric structure of optimal active sites. The method is illustrated on the oxygen reduction reaction catalyzed by platinum. Sites with the same number of first-nearest neighbors as (111) terraces but with an increased number of second-nearest neighbors are predicted to have superior catalytic activity. We used this rationale to create highly active sites on platinum (111), without alloying and using three different affordable experimental methods.
authors.affiliation: Université de Lyon, CNRS, École Normale Supérieure de Lyon, Université Claude Bernard Lyon 1, Laboratoire de Chimie, 46 Allée d'Italie, 69364 Lyon Cedex-07, France. Leiden Institute of Chemistry, Leiden University, Post Office Box 9502, 2300 RA Leiden, Netherlands. These authors contributed equally to this work. bandarenka@ph.tum.de philippe.sautet@ens-lyon.fr f.calle.vallejo@chem.leidenuniv.nl.
authors.forename: Federico
authors.initials: F
authors.lastname: Calle-Vallejo
authors.affiliation: Center for Electrochemical Sciences, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany. Analytical Chemistry, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany. These authors contributed equally to this work.
authors.forename: Jakub
authors.initials: J
authors.lastname: Tymoczko
authors.affiliation: Center for Electrochemical Sciences, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany. Energy Conversion and Storage, Physik-Department, Technische Universität München, James-Franck-Straße 1, 85748 Garching, Germany.
authors.forename: Viktor
authors.initials: V
authors.lastname: Colic
authors.affiliation: Physical Chemistry I, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany.
authors.forename: Quang Huy
authors.initials: QH
authors.lastname: Vu
authors.affiliation: Energy Conversion and Storage, Physik-Department, Technische Universität München, James-Franck-Straße 1, 85748 Garching, Germany.
authors.forename: Marcus D
authors.initials: MD
authors.lastname: Pohl
authors.affiliation: Physical Chemistry I, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany.
authors.forename: Karina
authors.initials: K
authors.lastname: Morgenstern
authors.affiliation: Université de Lyon, CNRS, École Normale Supérieure de Lyon, Université Claude Bernard Lyon 1, Laboratoire de Chimie, 46 Allée d'Italie, 69364 Lyon Cedex-07, France.
authors.forename: David
authors.initials: D
authors.lastname: Loffreda
authors.affiliation: Université de Lyon, CNRS, École Normale Supérieure de Lyon, Université Claude Bernard Lyon 1, Laboratoire de Chimie, 46 Allée d'Italie, 69364 Lyon Cedex-07, France. bandarenka@ph.tum.de philippe.sautet@ens-lyon.fr f.calle.vallejo@chem.leidenuniv.nl.
authors.forename: Philippe
authors.initials: P
authors.lastname: Sautet
authors.affiliation: Center for Electrochemical Sciences, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany. Analytical Chemistry, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany.
authors.forename: Wolfgang
authors.initials: W
authors.lastname: Schuhmann
authors.affiliation: Center for Electrochemical Sciences, Ruhr-Universität Bochum, Universitätstrasse 150, 44780 Bochum, Germany. Energy Conversion and Storage, Physik-Department, Technische Universität München, James-Franck-Straße 1, 85748 Garching, Germany. Nanosystems Initiative Munich, Schellingstraße 4, 80799 Munich, Germany. bandarenka@ph.tum.de philippe.sautet@ens-lyon.fr f.calle.vallejo@chem.leidenuniv.nl.
authors.forename: Aliaksandr S
authors.initials: AS
authors.lastname: Bandarenka