Challenges for the application of quantum chemical calculations to problems in catalysis

A long-standing goal of researchers in the field of catalysis is to develop first-principles methods for determining catalyst activity and selectivity. Advances in quantum chemical methods and codes, together with impressive improvements in computer speed, have contributed significantly towards the achievement of this objective. A review of current quantum chemical theories and models of catalytically active sites is presented with the aim of defining what is possible today and what needs to be done. Particular attention is given to identifying the trade-offs between achieving accurate energies of adsorbed and transition states and computational cost. Methods available for finding reaction pathways and calculating rate coefficients are also reviewed and discussed.