Towards the 4 V-class n-type organic lithium-ion positive electrode materials: the case of conjugated triflimides and cyanamides

Guo, Xiaolong;Apostol, Petru;Zhou, Xuan;Wang, Jiande;Vlad, Alexandru;et.al.
(2024) Energy & Environmental Science — Vol. 17, n° 1, p. 173-182 (2024)

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Abstract
Organic electrode materials have garnered a great deal of interest owing to their sustainability, cost-efficiency, and design flexibility metrics. Despite numerous endeavors to fine-tune their redox potential, the pool of organic positive electrode materials with a redox potential above 3 V versus Li+/Li0, and maintaining air stability in the Li-reservoir configuration remains limited. This study expands the chemical landscape of organic Li-ion positive electrode chemistries towards the 4 V-class through molecular design based on electron density depletion within the redox center via the mesomeric effect of electron-withdrawing groups (EWGs). This results in the development of novel families of conjugated triflimides and cyanamides as high-voltage electrode materials for organic lithium-ion batteries. These are found to exhibit ambient air stability and demonstrate reversible electrochemistry with redox potentials spanning the range of 3.1 V to 3.8 V (versus Li+/Li0), marking the highest reported values so far within the realm of n-type organic chemistries. Through comprehensive structural analysis and extensive electrochemical studies, we elucidate the relationship between the molecular structure and the ability to fine-tune the redox potential. These findings offer promising opportunities to customize the redox properties of organic electrodes, bridging the gap with their inorganic counterparts for application in sustainable and eco-friendly electrochemical energy storage devices.
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Guo, X., Apostol, P., Zhou, X., Wang, J., Lin, X., Darsi Rambabu, Du, M., Er, S., & Vlad, A. (2024). Towards the 4 V-class n-type organic lithium-ion positive electrode materials: the case of conjugated triflimides and cyanamides. Energy & Environmental Science, 17(1), 173-182. https://doi.org/10.1039/d3ee02897f (Original work published 2024)