Computational\nDecoration of Helicene for the Design\nof Graphene-like Anodes with Optimized Redox Activity

The electrochemical design of organic\ncompounds for eco-friendly\nnext-generation display devices and electrochemical energy storage\nsystems is crucial for improving performance. However, most efforts\nto enhance the charge/energy storage capabilities of anode materials\nin Li-ion batteries have concentrated on graphene and its derivatives,\noverlooking the potential of various organic compounds. In this study,\nwe employ an advanced computational protocol to design a series of\nhelicene-based graphene-like frameworks through functionalization\nand heteroatom doping. Incorporating selected functional groups or\ndopants into helicenes induces electron localization, influenced by\nthe electronic nature of the modifier (e.g., CNO ∼ COOH >\nCF<sub>3</sub>). This localization significantly enhances the redox\nactivities\nand intrinsic redox potentials of the helicenes, identifying candidates\nwithin our target redox potential range of 1.8–2.0 V vs Li/Li<sup>+</sup>. Further evaluation of selected candidates exhibiting intrinsic\nredox potentials within our target range as alternatives to graphene-based\nanodes reveals that 1,9,13,16,18-P-helicene stands out as the highest-performance\nanode material, with a theoretical charge capacity of 582.5 mAh/g\nand energy density of 696.1 mWh/g, while maintaining structural integrity\nduring the discharge process. Overall, our computational protocol\nemployed to design organic anode materials will advance the development\nof electrochemical energy storage devices and next-generation electronic\ndisplay technologies in terms of cell performance and environmental\nload.