| Abstract | The world’s energy systems will need to be changed radically if they are going to supply our energy needs in a sustainable manner over a long-term basis. Access to safe, clean, and sustainable energy supplies is one of the greatest challenges facing humanity during the twenty-first century. Energy from renewable resources – wind, water, the sun, and biomass – is inexhaustible and clean. Solar cells and electrochemical devices such as electrolyzers can be coupled with these intermittent power sources to store electricity in the form of chemical energy, in chemicals such as hydrogen, methanol, ethanol, and ethane (among others) for later use. Such processes have the potential to address the ever-increasing demand for chemicals and fuels while mitigating anthropogenic CO₂ emissions. Catalytic materials play an important role in these promising energy conversion technologies. Based initially on empirical approaches and chemical intuition, catalyst development has been fostered by combining physical and chemical models under the Sabatier’s principle, according to which the interactions between the catalyst and the substrate should be neither too strong nor too weak and “just right”. Recent developments of computational tools, such as density functional theory (DFT), have led to an unprecedented understanding of the materials properties and enabled predicting catalytic properties a priori. Catalyst discovery has been revolutionized as a result of rising computational capabilities and especially by the extensive use of DFT calculations, which provide a powerful computational framework to study catalytic reactions and identify new chemically active materials. In particular, combinatorial quantumchemical and high-throughput calculations have provided a powerful framework for the discovery of new catalysts. For example, DFT has provided the computational foundation of the hard and soft acid and base (HSAB) principle of Pearson and enabled the calculation of reactivity descriptors, such as hardness, softness, and Fukui functions. The d-band model developed by Nørskov and co-workers to relate the calculated adsorption energy to experimentally measurable catalytic properties. |
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