In Situ Electrochemical Activation of Hydroxyl Polymer Cathode for High-Performance Aqueous Zinc-Organic Batteries

Angew Chem Int Ed Engl. 2023 Aug 28;62(35):e202307365. doi: 10.1002/anie.202307365. Epub 2023 Jul 20.

Abstract

The slow reaction kinetics and structural instability of organic electrode materials limit the further performance improvement of aqueous zinc-organic batteries. Herein, we have synthesized a Z-folded hydroxyl polymer polytetrafluorohydroquinone (PTFHQ) with inert hydroxyl groups that could be partially oxidized to the active carbonyl groups through the in situ activation process and then undertake the storage/release of Zn2+ . In the activated PTFHQ, the hydroxyl groups and S atoms enlarge the electronegativity region near the electrochemically active carbonyl groups, enhancing their electrochemical activity. Simultaneously, the residual hydroxyl groups could act as hydrophilic groups to enhance the electrolyte wettability while ensuring the stability of the polymer chain in the electrolyte. Also, the Z-folded structure of PTFHQ plays an important role in reversible binding with Zn2+ and fast ion diffusion. All these benefits make the activated PTFHQ exhibit a high specific capacity of 215 mAh g-1 at 0.1 A g-1 , over 3400 stable cycles with a capacity retention of 92 %, and an outstanding rate capability of 196 mAh g-1 at 20 A g-1 .

Keywords: High Rate; Hydroxyl Polymer; In Situ Electrochemical Activation; Organic Electrodes; Zn-Ion Batteries.