Autonomous Reaction Network Exploration in Homogeneous and Heterogeneous Catalysis

Abstract

Autonomous computations that rely on automated reaction network elucidation algorithms may pave the way to make computational catalysis on a par with experimental research in the field. Several advantages of this approach are key to catalysis: (i) automation allows one to consider orders of magnitude more structures than what would be accessible by manual inspection, eventually with full resolution of structural varieties and conformations as well as with respect to the type and number of potentially important elementary reaction steps (including decomposition reactions that determine turnover number), (ii) fast electronic structure methods with uncertainty quantification warrant high efficiency and reliability in order to not only deliver results quickly, but also to allow for predictive work, and (iii) a high degree of autonomy reduces processing errors and human bias. In this work, we first review the state of the art in this research area, then discuss important conceptual issues that eventually determine feasibility and reliability of computational procedures, and finally demonstrate an implementation of these concepts applied to a catalytic system.