Bioinspired Catechol-Grafting PEDOT Cathode for an All-Polymer Aqueous Proton Battery with High Voltage and Outstanding Rate Capacity

Aqueous all-polymer proton batteries (APPBs) consisting of redox-active polymer electrodes are considered safe and clean renewable energy storage sources. However, there remain formidable challenges for APPBs to withstand a high current rate while maximizing high cell output voltage within a narrow electrochemical window of aqueous electrolytes. Here, a capacitive-type polymer cathode material is designed by grafting poly(3,4-ethylenedioxythiophene) (PEDOT) with bioinspired redox-active catechol pendants, which delivers high redox potential (0.60 V vs Ag/AgCl) and remarkable rate capability. The pseudocapacitive‑dominated proton storage mechanism illustrated by the density functional theory (DFT) calculation and electrochemical kinetics analysis is favorable for delivering fast charge/discharge rates. Coupled with a diffusion-type anthraquinone-based polymer anode, the APPB offers a high cell voltage of 0.72 V, outstanding rate capability (64.8% capacity retention from 0.5 to 25 A g−1), and cycling stability (80% capacity retention over 1000 cycles at 2 A g−1), which is superior to the state-of-the-art all-organic proton batteries. This strategy and insight provided by DFT and ex situ characterizations offer a new perspective on the delicate design of polymer electrode patterns for high-performance APPBs.