Regulating Intermolecular Hydrogen Bonds in Organic Cathode Materials to Realize Ultra‐stable, Flexible and Low‐temperature Aqueous Zinc‐organic Batteries

Rational design of molecular structures is one of the effective strategies to obtain high‐performance organic cathode materials. However, besides the optimization of single‐molecule structures, the influence of the "weak" interaction forces (e.g. hydrogen bonds) in organic cathode materials on the performance of batteries should be fully considered. Herein, three organic small molecules with different numbers of hydroxyl groups (namely nitrogen heterocyclic tetraketone (DAB), monohydroxyl nitrogen heterocyclic dione (HDA), dihydroxyl nitrogen heterocyclic dione (DHT)) were selected as the cathodes of aqueous zinc ion batteries (AZIBs), and the effect of the intermolecular hydrogen bonds on their electrochemical performance was studied for the first time. Clearly, the stable hydrogen‐bond networks built through the hydroxyl groups significantly enhance the cycle stability of organic small‐molecule cathodes and facilitate rapid proton conduction between the hydrogen‐bond networks through the Grotthuss mechanism, thereby endowing them with excellent rate performance. In addition, a larger and more dense two‐dimensional hydrogen‐bond network can be constructed through multiple hydroxyl groups, further enhancing the structural stability of organic small‐molecule cathodes, giving them better cycle tolerance, excellent rate performance, and extreme environmental tolerance.