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

Autor: Achazi AJ; Physikalisch-Chemisches Institut, Justus-Liebig-Universität Gießen, Gießen, Germany.; Zentrum für Materialforschung, Justus-Liebig-Universität Gießen, Gießen, Germany., Fataj X; Laboratory of Organic and Macromolecular Chemistry (IOMC), Friedrich Schiller University Jena, Jena, Germany.; Center for Energy and Environmental Chemistry Jena (CEEC Jena), Friedrich Schiller University Jena, Jena, Germany., Rohland P; Laboratory of Organic and Macromolecular Chemistry (IOMC), Friedrich Schiller University Jena, Jena, Germany.; Center for Energy and Environmental Chemistry Jena (CEEC Jena), Friedrich Schiller University Jena, Jena, Germany., Hager MD; Laboratory of Organic and Macromolecular Chemistry (IOMC), Friedrich Schiller University Jena, Jena, Germany.; Center for Energy and Environmental Chemistry Jena (CEEC Jena), Friedrich Schiller University Jena, Jena, Germany., Schubert US; Laboratory of Organic and Macromolecular Chemistry (IOMC), Friedrich Schiller University Jena, Jena, Germany.; Center for Energy and Environmental Chemistry Jena (CEEC Jena), Friedrich Schiller University Jena, Jena, Germany., Mollenhauer D; Physikalisch-Chemisches Institut, Justus-Liebig-Universität Gießen, Gießen, Germany.; Zentrum für Materialforschung, Justus-Liebig-Universität Gießen, Gießen, Germany.
Jazyk: angličtina
Zdroj: Journal of computational chemistry [J Comput Chem] 2024 May 30; Vol. 45 (14), pp. 1112-1129. Date of Electronic Publication: 2024 Jan 23.
DOI: 10.1002/jcc.27299
Abstrakt: 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.
(© 2024 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC.)
Databáze: MEDLINE