Computational Organometallic Catalysis: Where We Are, Where We Are Going

This essay gives my personal perspective of the current stage of computational methods applied to modeling organometallic catalysis, as well as the new directions the field is taking. The first part of the essay deals with what I consider the state‐of‐the‐art to build up energy profiles, regarding both chemical and computational models. With a proper choice of the chemical model and computational methods, quantum mechanical calculations are nowadays able to provide accurate energy profiles of organometallic reactions in solution involving closed‐shell species. However, in most cases they are still used to “predict the past”, providing after‐the‐fact explanations and missing out the full potential of contemporary simulation techniques. Simulations are mature enough to be incorporated at the design stage and to guide the experimental exploration. The new directions the field is taking, incorporating automated exploration methods and combined with extensive data analysis and machine learning algorithms, approach the holy grail of catalyst discovering. What makes current DFT calculations of organometallic reactions reliable? Are they efficiently employed? How do they connect with reaction mechanisms? How are they approaching the long‐sought catalyst design? Are theoreticians still needed? This essay collects my personal answers to these and other related questions.