Computational Design of Catalytic Materials for Fuels and Chemicals Production using Activity Descriptors

Heterogeneous catalysis is widely considered as one of the key technologies for a sustainable and CO2 neutral energy future, but new catalytic materials need to be discovered in order to achieve this goal. Over the past decades, the discovery of heterogeneous catalysts has been largely based on heuristics, trial-and-error approaches and combinatorial high-throughput experimentation. Recent advances in surface science techniques and density functional theory (DFT) simulations, however, have led to an unprecedented knowledge of the fundamental processes that govern the observed catalytic activity and selectivity. While a complete understanding of the often very complex reaction networks and the dynamically restructuring of the catalyst’s surface is still lacking, it is possible to make qualitative predictions about catalytic performance based on reactivity descriptors. Binding energies of key intermediates or the d-band center of transition metal catalysts are often well-suited to describe catalytic trends and can thereby reduce the complexity of the overall process to just a few variables.1,2 An overview of general computational catalyst design strategies will be presented and illustrated step-by-step on the example of the HCN synthesis reaction from CH4 and NH3 over transition metal surfaces.3 Our current efforts to extend this strategy to catalytic reactions at the significantly more complex interface between metals and metal-oxide supports will be briefly introduced using the prototypical CO oxidation reaction.4

REFERENCES
(1) Abild-Pedersen, F.; Greeley, J.; Studt, F.; Rossmeisl, J.; Munter, T. R.; Moses, P. G.; Skúlason, E.; Bligaard, T.; Nørskov, J. K. Phys. Rev. Lett. 2007, 99, 16104–16105.
(2) Wang, S.; Temel, B.; Shen, J.; Jones, G.; Grabow, L. C.; Studt, F.; Bligaard, T.; Abild-Pedersen, F.; Christensen, C. H.; Nørskov, J. K. Catal. Letters 2010, 141, 370–373.
(3) Grabow, L. C.; Studt, F.; Abild-Pedersen, F.; Petzold, V.; Kleis, J.; Bligaard, T.; Nørskov, J. K. Angew. Chemie Int. Ed. 2011, 50, 4601–4605.
(4) Saavedra, J.; Doan, H. A.; Pursell, C. J.; Grabow, L. C.; Chandler, B. D. Science 2014, 345, 1599–1602.