Interlocking-driven and hydrogen-bond mediated molecular constraints toward high-rate and durable quinonoid polymer cathode for aqueous Zn-organic batteries

Quinonoid polymer cathodes demonstrate great promise for aqueous zinc ion batteries (AZIBs) owing to their sustainability and structural diversity. However, their unavoidable dissolution and sluggish redox kinetics severely limit their practical application in AZIBs. Herein, we propose a multiple interlocking strategy through constructing an integrated network of a juglone/carbon nanotube composite interconnected with sodium polyacrylate (PAANa) binder (J@CNT-PAANa). The synergistic hydrogen-bonding, π − π stacking, and conductive network in J@CNT-PAANa enable robust adhesion, simultaneously enhancing structural stability and suppressing juglone dissolution. The robust π-π stacking with CNT provides physical confinement, while the hydrogen bonding with PAANa offers strong chemical anchoring. Together, they synergistically construct a stable network that suppresses dissolution and enhances interfacial stability. Compared to conventional binders, PAANa exhibits superior binding energy when serving as a binder with juglone, coupled with enhanced adhesion, dispersibility, wettability, and mechanical flexibility, enabling exceptional interfacial stability and ion diffusion capability in J@CNT cathode. Leveraging dual constraints from physical interlocking and hydrogen bond networks, J@CNT cathode with the PAANa binder delivers a reversible capacity of 178 mAh g⁻¹ at 0.1 A g⁻¹. At 0.5 A g⁻¹, J@CNT-PAANa maintains 110 mAh g⁻¹ after 2000 cycles, corresponding to 80.1 % capacity retention. This performance represents 125 %, 134 %, and 237 % higher capacities compared to CMC, SA, and PVDF-based electrodes, respectively. Furthermore, PAANa binder can participate in forming a co-constructed cathode-electrolyte interface layer, further boosting mechanical stability. This research provides a new understanding of the water-soluble binders on organic electrode in aqueous Zn-organic batteries systems.