Computational Decoration of Helicene for the Design of Graphene-like Anodes with Optimized Redox Activity

Abstract

The electrochemical design of organic compounds for eco-friendly next-generation display devices and electrochemical energy storage systems is crucial for improving performance. However, most efforts to enhance the charge/energy storage capabilities of anode materials in Li-ion batteries have concentrated on graphene and its derivatives, overlooking the potential of various organic compounds. In this study, we employ an advanced computational protocol to design a series of helicene-based graphene-like frameworks through functionalization and heteroatom doping. Incorporating selected functional groups or dopants into helicenes induces electron localization, influenced by the electronic nature of the modifier (e.g., CNO ∼ COOH > CF 3 ). This localization significantly enhances the redox activities and intrinsic redox potentials of the helicenes, identifying candidates within our target redox potential range of 1.8−2.0 V vs Li/Li + . Further evaluation of selected candidates exhibiting intrinsic redox potentials within our target range as alternatives to graphenebased anodes reveals that 1,9,13,16,18-P-helicene stands out as the highest-performance anode material, with a theoretical charge capacity of 582.5 mAh/g and energy density of 696.1 mWh/g, while maintaining structural integrity during the discharge process. Overall, our computational protocol employed to design organic anode materials will advance the development of electrochemical energy storage devices and next-generation electronic display technologies in terms of cell performance and environmental load.