Metal-free aqueous batteries offer environmentally friendly energy storage without depleting the global reserves of strategic elements. These batteries consist of solid, redox-active polymeric anodes and cathodes with a water-based electrolyte. However, the performance of available active polymers remains inferior, and design principles to guide future development are lacking. Here, we report on the coupled mass, electron, and water transfer behavior for a series of non-conjugated nitroxide radical polymers in a water-based electrolyte-containing organic salt for guiding future design. In situ monitoring of the charge-discharge process reveals the important role of polymer-water interactions. Specifically, improved polymer-water interactions manifest in accelerated kinetics, which promote capacity retention at higher discharge rates. The most hydrophilic polymer, poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl acrylamide) (PTAm), yielded a capacity of 115 mAh/g, or 97% of its theoretical value, at 0.05 mA/cm². At 5 mA/cm², the PTAm capacity remained relatively high at 50 mAh/g, whereas comparable polymer capacities were much lower.

无金属水性电池可提供环保的能量存储，而不会耗尽全球战略元素的储备。这些电池由固态，具有氧化还原活性的聚合物阳极和带有水基电解质的阴极组成。然而，可用的活性聚合物的性能仍然较差，并且缺乏指导未来发展的设计原理。在这里，我们报告了一系列非共轭氮氧化物自由基聚合物在水基含电解质的有机盐中的耦合质量，电子和水传递行为，以指导未来的设计。原位充放电过程的监测揭示了聚合物与水相互作用的重要作用。具体而言，改进的聚合物与水的相互作用表现为加速的动力学，这促进了较高放电速率下的容量保持。亲水性最高的聚合物，聚（2,2,6,6-四甲基哌啶基氧基-4-基丙烯酰胺）（PTAm）在0.05 mA / cm ²的容量为115 mAh / g，或理论值的97％。在5 mA / cm ^2时，PTAm容量保持相对较高，为50 mAh / g，而可比的聚合物容量则低得多。