Autonomous Reaction Network Exploration in Homogeneous and Heterogeneous Catalysis

TL;DR

This paper discusses the development of autonomous computational methods for reaction network exploration in catalysis, enabling systematic, unbiased, and efficient analysis of complex catalytic processes with potential for new discoveries.

Contribution

It introduces a framework for autonomous reaction network exploration in catalysis, integrating fast electronic structure methods and addressing conceptual challenges.

Findings

Automated exploration can consider vastly more structures than manual methods.

High efficiency and reliability enable predictive catalysis modeling.

Autonomous methods facilitate unbiased, high-fidelity analysis with potential for surprising discoveries.

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 in a systematic and open-ended fashion than what would be accessible by manual inspection. Eventually, full resolution in terms 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 numbers) may be achieved. (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. (iii) A high degree of autonomy reduces the amount of manual human work, processing errors, and human bias. Although being inherently unbiased, it is still steerable with respect to specific regions of an emerging network and with respect to the addition of new reactant species. This allows for a high fidelity of the formalization of some catalytic process and for surprising in silico discoveries. In this work, we first review the state of the art in computational catalysis to embed autonomous explorations into the general field from which it draws its ingredients. We then elaborate on the specific conceptual issues that arise in the context of autonomous computational procedures, some of which we discuss at an example catalytic system.