Journal article

Authors list: Achazi, Andreas J; Fataj, Xhesilda; Rohland, Philip; Hager, Martin D; Schubert, Ulrich S; Mollenhauer, Doreen

Publication year: 2024

Pages: 1112-1129

Journal: Journal of Computational Chemistry

Volume number: 45

Issue number: 14

ISSN: 0192-8651

eISSN: 1096-987X

Open access status: Hybrid

DOI Link: https://doi.org/10.1002/jcc.27299

Publisher: Wiley

Abstract: 

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.

Harvard Citation style: Achazi, A., Fataj, X., Rohland, P., Hager, M., Schubert, U. and Mollenhauer, D. (2024) Development of a multi-step screening procedure for redox active molecules in organic radical polymer anodes and as redox flow anolytes, Journal of Computational Chemistry, 45(14), pp. 1112-1129. https://doi.org/10.1002/jcc.27299

APA Citation style: Achazi, A., Fataj, X., Rohland, P., Hager, M., Schubert, U., & Mollenhauer, D. (2024). Development of a multi-step screening procedure for redox active molecules in organic radical polymer anodes and as redox flow anolytes. Journal of Computational Chemistry. 45(14), 1112-1129. https://doi.org/10.1002/jcc.27299