Vesicular-like manganese single-atom doped Poly(1,5-Naphthalenediamine) cathode for durable bipolar zinc-organic batteries

Abstract

Traditional polymers often encounter capacity limitations due to their low active unit density and suboptimal operating voltages (<1 V vs. Zn/Zn²⁺). In contrast, bipolar polymers, which integrate the advantages of both n- and p-type polymers, offer the potential to create superior zinc-organic batteries (ZOBs). In this study, we report on a novel bipolar poly(1,5-Naphthalenediamine) cathode material doped with manganese single atoms (MnSA@PN), where C=N/C-N redox sites participate in electron transfer processes, serving as storage sites for both cations and anions. Importantly, MnSA@PN features a unique nanovesicle structure that enhances electrolyte permeability, thereby shortening the ion diffusion pathway. Therefore, the Zn//MnSA@PN full battery demonstrates high capacity (259 mAh g⁻¹ at 0.1 A g⁻¹), an elevated average voltage (1.6 V), and exceptional energy density (185 Wh kg⁻¹). This work broadens the electrochemical prospects of bipolar polymers, positioning them as promising materials for cutting-edge ZOBs.