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Evaluation of Computational Chemistry Methods for Predicting Redox Potentials of Quinone-Based Cathodes for Li-Ion Batteries

High-throughput computational screening (HTCS) is an effective tool to accelerate the discovery of active materials for Li-ion batteries. For the evaluation of organic cathode materials, the effectiveness of HTCS depends on the accuracy of the employed chemical descriptors and their computing cost. This work was focused on evaluating the performance of computational chemistry methods, including semi-empirical quantum mechanics (SEQM), density-functional tight-binding (DFTB), and density functional theory (DFT), for the prediction of the redox potentials of quinone-based cathode materials for Li-ion batteries. In addition, we evaluated the accuracy of three energy-related descriptors: (1) the redox reaction energy, (2) the lowest unoccupied molecular orbital (LUMO) energy of reactant molecules, and (3) the highest occupied molecular orbital (HOMO) energy of lithiated product molecules. Among them, the LUMO energy of the reactant compounds, regardless of the level of theory used for its calculation, showed the best performance as a descriptor for the prediction of experimental redox potentials. This finding contrasts with our earlier results on the calculation of quinone redox potentials in aqueous media for redox flow batteries, for which the redox reaction energy was the best descriptor. Furthermore, the combination of geometry optimization using low-level methods (e.g., SEQM or DFTB) followed by energy calculation with DFT yielded accuracy as good as the full optimization of geometry using the DFT calculations. Thus, the proposed calculation scheme is useful for both the optimum use of computational resources and the systematic generation of robust calculation data on quinone-based cathode compounds for the training of data-driven material discovery models.