Unveiling Activation Process of C═N Cathode for High‐Performing Zinc‐Organic Batteries

Zinc‐organic batteries (ZOBs) based on C═N compounds arouse great interest due to wide structure, high capacity, and long cycle life. However, activation phenomenon of C═N compound is seldom discussed in ZOBs, as well as activation mechanism during charging/discharging. Herein, DPPT (Diphenazine‐pyrenetetraimine) with eight C═N active sites is first synthesized for ZOBs, delivering ultralong cycling life (45 000 cycles) and good rate performance (20 C). Notably, there shows obvious activation process at beginning cycles because of the transformation of DPPT‐eight proton into DPPT. In situ experiments and DFT calculations reveal co‐participation mechanism of Zn 2+ & H + with optimized structure of 2DPPT‐1Zn‐14H deriving from 16 discharged products. Impressively, wearable NH 3 sensors could be powered by as‐fabricated flexible DPPT ZOBs, making it possible from the restriction of traditional power supply. Prospectively, activation mechanism of high‐performing DPPT would provide methods for further design of organic structures into ZOBs and offer self‐powered energy for wearable sensors.