Effects of Conjugated Structure on the Magnesium Storage Performance of Dianhydrides

Abstract Inorganic cathodes of rechargeable Mg batteries suffer from limited selections, while organic materials provide more options. Herein, three conjugated dianhydrides, pyromellitic dianhydride, 1,4,5,8‐naphthalenetetracarboxylic dianhydride and 3,4,9,10‐perylenetetracarboxylic dianhydride are comparatively investigated to elucidate the effects of conjugated structure on the Mg 2+ storage performances. It is observed that the reversible Mg 2+ storage capacity is more dependent on the conjugated structure than carbonyl numbers. Ex‐situ mechanism study illustrates that the extended conjugated structure delocalizes the electron density, hence enhancing carbonyl enolization and increasing the Mg 2+ storage capacity. Furthermore, the largely conjugated structure buffers the charge density change during repeated magnesiation/demagnesiation resulting in better cyclability. Prominently, 3,4,9,10‐perylenetetracarboxylic dianhydride shows a high Mg 2+ storage capacity (160 mAh g −1 ) and a good cycling stability (80 % capacity retention after 100 cycles) with the largest conjugated structure. This work provides a low‐cost cathode for rechargeable Mg batteries that can be utilized for designing high‐performance organic Mg battery cathodes.