Self‐Charging Aqueous Zn//COF Battery with UltraHigh Self‐Charging Efficiency and Rate

Self-charging zinc batteries that combine energy harvesting technology with batteries are candidates for reliable self-charging power systems. However, the lack of rational materials design results in unsatisfactory self-charging performance. Here, a covalent organic framework containing pyrene-4,5,9,10-tetraone groups (COF-PTO) is reported as a cathode material for aqueous self-charging zinc batteries. The ordered channel structure of the COF-PTO provides excellent capacity retention of 98% after 18 000 cycles at 10 A g^-1 and ultra-fast ion transfer. To visually assess the self-charging performance, two parameters, namely self-charging efficiency (self-charging discharge capacity/galvanostatic discharge capacity, η) and average self-charging rate (total discharge capacity after cyclic self-charging/total cyclic self-charging time, ν), are proposed for performance evaluation. COF-PTO achieves an impressive η of 96.9% and an ν of 30 mAh g^-1 self-charge capacity per hour in 100 self-charging cycles, surpassing the previous reports. Mechanism studies reveal the co-insertion of Zn²⁺ and H⁺ double ions in COF-PTO of self-charging zinc batteries. In addition, the C═N and C═O (on the benzene) in COF-PTO are ortho structures to each other, which can easily form metal heterocycles with Zn ions, thereby driving the forward progress of the self-charging reaction and enhancing the self-charging performance.