Multi-Objective Goal-Directed Optimization of De Novo Stable Organic Radicals for Aqueous Redox Flow Batteries

Shree Sowndarya S. V., Jeffrey Law, Charles Tripp, Dmitry Duplyakin, Erotokritos Skordilis, David Biagioni, Robert S. Paton, Peter St. John

Research output: Contribution to journalArticlepeer-review

34 Scopus Citations

Abstract

Advances in the field of goal-directed molecular optimization offer the promise of finding feasible candidates for even the most challenging molecular design applications. One example of a fundamental design challenge is the search for novel stable radical scaffolds for an aqueous redox flow battery that simultaneously satisfy redox requirements at the anode and cathode, as relatively few stable organic radicals are known to exist. To meet this challenge, we develop a new open-source molecular optimization framework based on AlphaZero coupled with a fast, machine-learning-derived surrogate objective trained with nearly 100,000 quantum chemistry simulations. The objective function comprises two graph neural networks: one that predicts adiabatic oxidation and reduction potentials and a second that predicts electron density and local three-dimensional environment, previously shown to be correlated with radical persistence and stability. With no hard-coded knowledge of organic chemistry, the reinforcement learning agent finds molecule candidates that satisfy a precise combination of redox, stability and synthesizability requirements defined at the quantum chemistry level, many of which have reasonable predicted retrosynthetic pathways. The optimized molecules show that alternative stable radical scaffolds may offer a unique profile of stability and redox potentials to enable low-cost symmetric aqueous redox flow batteries.

Original languageAmerican English
Pages (from-to)720-730
Number of pages11
JournalNature Machine Intelligence
Volume4
DOIs
StatePublished - 2022

Bibliographical note

Publisher Copyright:
© 2022, The Author(s).

NREL Publication Number

  • NREL/JA-2700-82096

Keywords

  • density functional theory
  • machine learning
  • organic radical chemistry
  • redox flow battery

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