Towards the 4 V-class n-type organic lithium-ion positive electrode materials: the case of conjugated triflimides and cyanamides
文献情報
Xiaolong Guo, Petru Apostol, Xuan Zhou, Jiande Wang, Xiaodong Lin, Darsi Rambabu, Mengyuan Du, Süleyman Er, Alexandru Vlad
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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