Journal of Catalysis 239 (2006) 501–506 www.elsevier.com/locate/jcat Research Note Toward computational screening in heterogeneous catalysis: Pareto-optimal methanation catalysts Martin P. Andersson a , Thomas Bligaard a , Arkady Kustov b , Kasper E. Larsen c , Jeffrey Greeley a , Tue Johannessen c , Claus H. Christensen b , Jens K. Nørskov a,∗ a Center for Atomic-Scale Materials Physics, Department of Physics, NanoDTU, Technical University of Denmark, DK-2800 Lyngby, Denmark b Center for Sustainable and Green Chemistry, Department of Chemistry, NanoDTU, Technical University of Denmark, DK-2800 Lyngby, Denmark c Department of Chemical Engineering, NanoDTU, Technical University of Denmark, DK-2800 Lyngby, Denmark Received 20 January 2006; revised 13 February 2006; accepted 18 February 2006 Available online 24 March 2006 Abstract Finding the solids that are the best catalysts for a given reaction is a daunting task due to the large number of combinations and structures of multicomponent surfaces. In addition, it is not only the reaction rate that needs to be optimized; the selectivity, durability, and cost must also be taken into account. Here we propose a computational screening approach and apply it to design a new metal alloy catalyst for the methanation reaction (CO + 3H 2 → CH 4 + H 2 O).  2006 Elsevier Inc. All rights reserved. Keywords: Alloy; Bimetallic; Methanation; Hydrogenation; Fischer–Tropsch; DFT; Design; Screening; Optimization; Pareto 1. Introduction It has been shown that the kinetics of full catalytic reac- tions can be described semiquantitatively on the basis of ther- mochemistry and activation energies calculated using density functional theory (DFT) [1–3]. If such an approach could be ex- tended from a single catalyst to a range of catalysts, then DFT calculations could be used for a first screening of new catalysts. Although this is not yet possible, we take a step in that direction with the following procedure. First, we establish a correlation between the catalytic activity and a descriptor, which we can calculate directly using DFT. The descriptor is chosen on the basis of a general understanding of parameters determining the variation in catalytic activity from one catalyst to the next [4,5]. We use experimental data for the activity of a set of elemental metals to determine the optimum value of the descriptor. Next, * Corresponding author. Fax: +45 45 93 23 99. E-mail address: norskov@fysik.dtu.dk (J.K. Nørskov). we perform a preliminary screening of a number of intermetal- lic alloys based on a model of the effect of alloying developed from DFT calculations. Then we study the most interesting al- loys using full DFT calculations to verify the alloy model and make definite predictions of the activity. Finally, we synthesize the best catalyst candidates and measure their catalytic activi- ty. To illustrate this approach, we use the methanation reac- tion (CO + 3H 2 → CH 4 + H 2 O). This is one of the classic reactions in heterogeneous catalysis [6–9] used in connection with, for instance, catalytic ammonia synthesis (N 2 + 3H 2 → 2NH 3 ) to remove trace amounts of CO from the hydrogen feed gas. It has attracted renewed interest for the clean up of reformate hydrogen fuels for low-temperature fuel cells in which CO is a strong poison [10]. The traditional metha- nation catalyst is Ni supported on Al 2 O 3 [9]. The reaction is well described experimentally [11,12] and theoretically [5, 13,14], and recently experimental high-throughput screening methods have been applied to find new catalysts for this reac- tion [15]. 0021-9517/$ – see front matter  2006 Elsevier Inc. All rights reserved. doi:10.1016/j.jcat.2006.02.016