Computational catalysis for sustainable chemistry: from reaction mechanisms to working devices
Evgeny A. PidkoInorganic
Materials Chemistry group and Institute for Complex Molecular Systems, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven
The transfer to sustainable energy and chemistry technologies is one of the important challenges for humanity in the 21st century. In a carbon-constrained economy, CO2 is expected to become an increasingly important source of carbon for chemical industry. In a transition period, the development of more sustainable processes based on natural gas and biomass as a feedstock are required. Catalysis plays a pivotal role in all chemical strategies towards novel more efficient and sustainable processes. They require new more active and selective catalysts for the production of useful chemicals from alternative feedstocks. So far, most developments in catalysis have been largely based on trial-and-error approaches. The grand challenge in the field is to make a step towards the rational design of efficient catalysts for a given chemical reaction. To progress in this direction it is imperative to learn how catalysts promote chemical transformations and how their performance can be controlled.
In this lecture, I will show how modern computational chemistry can provide such information and thus create a foundation for the rational catalyst design. Several examples from my recent studies on catalytic C1 chemistry will be discussed. The main focus will be on such processes as the direct oxidation of methane, Ni-catalyzed synthesis of acrylates via CO2 coupling with ethylene and the reversible hydrogenation of CO2 by Ru pincer catalysts. With these examples, I will illustrate how theoretical calculations complemented by dedicated experiments can help creating a molecularly resolved picture of complex catalytic processes and how this knowledge can guide the development of new and improved catalytic systems, which create a basis for engineering innovative technological solutions.
 (a) S. Grundner, M.A.C. Markovits, G. Li, M. Tromp, E.A. Pidko, E.J.M. Hensen, A. Jentys, M. Sanchez-Sanchez, J.A. Lercher, Nat. Commun. 2015, 6, 7546; (b) G. Li, P. Vassilev, M. Sanchez-Sanchez, J.A. Lercher, E.J.M. Hensen, E.A. Pidko, J. Catal. 2016, 338, 305.
 (a) G. Yang, B. Schäffner, M. Blug, E.J.M. Hensen, E.A. Pidko, ChemCatChem 2014, 6, 800; 2; (b) C. Hendriksen, E.A. Pidko, G. Yang, B. Schäffner, D. Vogt, Chem. Eur. J. 2014, 20, 12037.
 (a) G.A. Filonenko, E.J.M. Hensen, E.A. Pidko, Catal. Sci. Technol. 2014, 4, 3474; (b) G.A. Filonenko, R. van Putten, E.N. Schulpen, E. Hensen, E.A. Pidko, ChemCatChem 2014, 6, 1526; (c) G.A. Filonenko, D. Smykowski, B.M. Szyja, E.J.M. Hensen, E.A. Pidko, ACS Catal. 2015, 5, 1145.