Pyrenetetrone Derivatives Tailored by Nitrogen Dopants for High-Potential Cathodes in Lithium-Ion Batteries
2019
Summary To overcome limited information on organic cathode materials for lithium-ion batteries, we study the electrochemical redox properties of pyrenetetrone and its nitrogen-doped derivatives. Three primary conclusions are highlighted from this study. First, the redox potential increases as increasing the number of electron-withdrawing nitrogen dopants. Second, the redox potentials of pyrenetetrone derivatives continuously decrease with the number of bound Li atoms during the discharging process due to the decrease in the reductive ability until the compounds become cathodically deactivated exhibiting negative redox potentials. Notably, pyrenetetrone with four nitrogen dopants loses its cathodic activity after the binding of five Li atoms, indicating remarkably high performance (496 mAh/g and 913 mWh/g). Last, the redox potential is strongly correlated not only with electronic properties but also with solvation energy. This highlights that pyrenetetrone derivatives would follow two-stage transition behaviors during the discharging process, implying a crucial contribution of solvation energy to their cathodic deactivation.
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