Development of a multi-step screening procedure for redox active molecules in organic radical polymer anodes and as redox flow anolytes

Development of a multi-step screening procedure for redox active molecules in organic radical polymer anodes and as redox flow anolytes

© 2024 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC.

Bibliographische Detailangaben
Veröffentlicht in:Journal of computational chemistry. - 1984. - 45(2024), 14 vom: 30. Apr., Seite 1112-1129
1. Verfasser: Achazi, Andreas J (VerfasserIn)
Weitere Verfasser: Fataj, Xhesilda, Rohland, Philip, Hager, Martin D, Schubert, Ulrich S, Mollenhauer, Doreen
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Journal of computational chemistry
Schlagworte:Journal Article DFT multi‐step screening organic redox flow battery polymer‐based batteries viologen
Beschreibung
Zusammenfassung:© 2024 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC.
Benzo[d]-X-zolyl-pyridinyl (XO, S, NH) radicals represent a promising class of redox-active molecules for organic batteries. We present a multistep screening procedure to identify the most promising radical candidates. Experimental investigations and highly correlated wave function-based calculations are performed to determine benchmark redox potentials. Based on these, the accuracies of different methods (semi-empirical, density functional theory, wave function-based), solvent models, dispersion corrections, and basis sets are evaluated. The developed screening procedure consists of three steps: First, a conformer search is performed with CREST. The molecules are selected based on the redox potentials calculated using GFN2-xTB. Second, HOMO energies calculated with reparametrized B3LYP-D3(BJ) and the def2-SVP basis set are used as selection criteria. The final molecules are selected based on the redox potentials calculated from Gibbs energies using BP86-D3(BJ)/def2-TZVP. With this multistep screening approach, promising molecules can be suggested for synthesis, and structure-property relationships can be derived
Beschreibung:Date Revised 12.04.2024
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1096-987X
DOI:10.1002/jcc.27299