Abstract
Organic cathode materials are attractive candidates for the development of high-performance Li-ion batteries (LIBs). The chemical space of candidate molecules is too vast to be explored solely by experiments; however, it can be systematically explored by a high-throughput computational search that incorporates a spectrum of screening techniques. Here, we present a time- and resource-efficient computational scheme that incorporates machine learning and semi-empirical quantum mechanical methods to study the chemical space of approximately 200 000 quinone-based molecules for use as cathode materials in LIBs. By performing an automated search on a commercial vendor database, computing battery-relevant properties such as redox potential, gravimetric charge capacity, gravimetric energy density, and synthetic complexity score, and evaluating the structural integrity upon the lithiation process, a total of 349 molecules were identified as potentially high-performing cathode materials for LIBs. The chemical space of the screened candidates was visualized using dimensionality reduction methods with the aim of further downselecting the best candidates for experimental validation. One such directly purchasable candidate, 1,4,9,10-anthracenetetraone, was analyzed through cyclic voltammetry experiments. The measured redox potentials of the two lithiation steps, , of 3.3 and 2.4 V, were in good agreement with the predicted redox potentials, , of 3.2 and 2.3 V vs. Li/Li(+), respectively. Lastly, to lay out the principles for rational design of quinone-based cathode materials beyond the current work, we constructed and discussed the quantitative structure property relationships of quinones based on the data generated from the calculations.