Due to the unique “Grotthus mechanism” of the proton as the charge carrier, aqueous proton batteries (APBs) have the potential to become a type of feasible energy storage device with low cost and high security. Organic polymers with tunable molecule structures are promising for APB electrodes, whereas unsatisfactory redox capacity and low electron affinity hinder their real applications. Herein, a highly redox-active polymer, poly(diquinoxalino-phenazine) (PDQPZ), has been designed and synthesized with extended imine-conjugated polymeric backbones. Beneficial from the reasonable molecular configuration, the PDQPZ polymer shows extensive electron delocalization and optimized molecular orbitals with an extremely small LUMO value of −3.26 eV, leading to excellent electron affinity and high redox activity for fast, ultra-stable and extraordinary proton storage, which are further demonstrated by localized orbital locator-π (LOL-π) and iso-chemical shielding surface (ICSS) techniques. As such, the PDQPZ polymer as electrode material possesses a superior proton-storage capacity of 205.2 mAh g⁻¹ and excellent cycling stability after 10,000 cycles with as low as 0.0008% decline per cycle. Multiple in-operando monitoring techniques further confirm highly reversible proton uptake/removal and the protonation pathways are proposed in detail. Finally, a high-performance and long-life APB device has been fabricated and operated over a wide temperature range.

由于质子作为电荷载体的独特“格罗特斯机制”，水质质子电池（APB）有潜力成为一种可行的低成本、高安全性的储能装置。具有可调节分子结构的有机聚合物有望用于APB电极，但不令人满意的氧化还原能力和低电子亲和力阻碍了其实际应用。在此，设计并合成了一种具有扩展亚胺共轭聚合物主链的高氧化还原活性聚合物聚（二喹喔啉-吩嗪）（PDQPZ）。受益于合理的分子构型，PDQPZ聚合物表现出广泛的电子离域和优化的分子轨道，其LUMO值极小为-3.26 eV，从而具有优异的电子亲和力和高氧化还原活性，可快速、等化学屏蔽表面（ICSS）技术。因此，作为电极材料的PDQPZ聚合物具有205.2mAh g ^-1的优异质子存储容量和10,000次循环后优异的循环稳定性，每次循环下降率低至0.0008%。多种操作中监测技术进一步证实了高度可逆的质子吸收/去除，并详细提出了质子化途径。最终，我们制造出了高性能、长寿命的 APB 器件，并可在较宽的温度范围内运行。