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Machine learning in chemical reaction space.

Published version
Peer-reviewed

Type

Article

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Abstract

Chemical compound space refers to the vast set of all possible chemical compounds, estimated to contain 1060 molecules. While intractable as a whole, modern machine learning (ML) is increasingly capable of accurately predicting molecular properties in important subsets. Here, we therefore engage in the ML-driven study of even larger reaction space. Central to chemistry as a science of transformations, this space contains all possible chemical reactions. As an important basis for 'reactive' ML, we establish a first-principles database (Rad-6) containing closed and open-shell organic molecules, along with an associated database of chemical reaction energies (Rad-6-RE). We show that the special topology of reaction spaces, with central hub molecules involved in multiple reactions, requires a modification of existing compound space ML-concepts. Showcased by the application to methane combustion, we demonstrate that the learned reaction energies offer a non-empirical route to rationally extract reduced reaction networks for detailed microkinetic analyses.

Description

Keywords

3404 Medicinal and Biomolecular Chemistry, 34 Chemical Sciences

Journal Title

Nat Commun

Conference Name

Journal ISSN

2041-1723
2041-1723

Volume Title

11

Publisher

Springer Science and Business Media LLC