期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 24, 期 26, 页码 16207-16219出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cp01717b
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资金
- Austrian Science Foundation (FWF) [Z222-N19]
- FWF [P29645, P34233]
- Leopold-Franzens-University of Innsbruck
- Austrian Science Fund (FWF) [P34233, P29645] Funding Source: Austrian Science Fund (FWF)
In this study, the electrochemical properties of anthraquinone and its derivatives were investigated using experimental data and computational methods. It was found that a low-cost method can be used for efficient pre-screening of candidate structures for organic electronic materials, followed by refinement using DFT methods to search for new high-performance materials.
Anthraquinone (AQ) has long been identified as a highly promising lead structure for various applications in organic electronics. Considering the enormous number of possible substitution patterns of the AQ lead structure, with only a minority being commercially available, a systematic experimental screening of the associated electrochemical potentials represents a highly challenging and time consuming task, which can be greatly enhanced via suitable virtual pre-screening techniques. In this work the calculated electrochemical reduction potentials of pristine AQ and 12 hydroxy- or/and amino-substituted AQ derivatives in N,N-dimethylformamide have been correlated against newly measured experimental data. In addition to the calculations performed using density functional theory (DFT), the performance of different semi-empirical density functional tight binding (DFTB) approaches has been critically assessed. It was shown that the SCC DFTB/3ob parametrization in conjunction with the COSMO solvation model provides a highly adequate description of the electrochemical potentials also in the case of the two-fold reduced species. While the quality in the correlation against the experimental data proved to be slightly inferior compared to the employed DFT approach, the highly advantageous cost-accuracy ratio of the SCC DFTB/3ob/COSMO framework has important implications in the formulation of hierarchical screening strategies for materials associated with organic electronics. Based on the observed performance, the low-cost method provides sufficiently accurate results to execute efficient pre-screening protocols, which may then be followed by a DFT-based refinement of the best candidate structures to facilitate a systematic search for new, high-performance organic electronic materials.
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