Discovery of lead low-potential radical candidates for organic radical polymer batteries with machine-learning-assisted virtual screening

The discovery and development of new low reduction potential molecules that also have fast charge transfer kinetics is necessary for the further development of organic redox-active polymers in practical battery applications. Theoretical methods can aid in finding the lead radical candidates in large...

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Bibliographic Details
Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2022-04, Vol.1 (15), p.8273-8282
Main Authors: Li, Cheng-Han, Tabor, Daniel P
Format: Article
Language:English
Subjects:
Batteries
Candidates
Charge transfer
Chemical fingerprinting
Coupling (molecular)
Electrode potentials
Gaussian process
Low cost
Machine learning
Polymers
Quantum chemistry
Radicals
Regression models
Screening
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Summary:The discovery and development of new low reduction potential molecules that also have fast charge transfer kinetics is necessary for the further development of organic redox-active polymers in practical battery applications. Theoretical methods can aid in finding the lead radical candidates in large initial screening spaces, but low-cost (yet accurate) methods are needed to predict the functional properties of the materials. In this paper, we conduct a two-objective (potential and dimer electronic coupling) virtual screening campaign to identify lead low potential candidate molecules in an initial space of 660 candidate molecules. The screening is accelerated by employing a trained Gaussian Process regression model for the voltage screening task. The model takes a combination of core-group chemical fingerprints and low-cost semi-empirical quantum chemistry calculations as the features for the model. The top-10%-predicted lowest reduction potential molecules of the initial space are then screened further to identify the candidates with the highest predicted electronic coupling. From the screening campaign, a set of promising redox-active molecules and two Pareto-optimal molecules (both N -methylphthalimides) are identified. Lead candidate radicals for use in radical polymer batteries are discovered by virtual screening with low computational footprint, chemistry-informed machine learning methods.
ISSN:2050-7488
2050-7496
DOI:10.1039/d2ta00743f