Graphitic Nitrogen-Regulated Direct I2/I− Conversion to Achieve Fast Kinetics and Stability for Zn–I2 Batteries

Iodine (I 2 ) cathodes for aqueous Zn–I 2 batteries suffer from sluggish redox kinetics and severe polyiodide shuttling, resulting in poor utilization and cycling stability. Herein, graphitic nitrogen-enriched carbonized polymer dots (CPDs) with a core–shell structure are integrated with a self-supporting porous carbon framework to construct a graphitic nitrogen-regulated porous carbon host. The porous framework provides abundant space for iodine accommodation and accessible pathways for mass transport, while CPDs introduce graphitic-N sites that strengthen iodine–host interactions and facilitate interfacial electron transfer. Their cooperative action favors a dominant direct I 2 /I − conversion pathway with substantially suppressed accumulation of soluble polyiodide species, thereby enabling fast iodine redox kinetics and excellent cycling stability. Benefiting from these synergistic effects, the optimized PCF-CPDs/I 2 -0.2 cathode delivers a high specific capacity of 146.1 mAh g −1 at 0.3 A g −1 with 99.6% capacity retention over 500 cycles. At 1 A g −1 , it maintains 117.5 mAh g −1 with 87.1% retention after 4000 cycles. This work demonstrates that coupling porous confinement with CPDs-mediated interfacial regulation provides an effective strategy for developing high-performance Zn–I 2 batteries. Graphical Graphitic-N-enriched carbonized polymer dots (CPDs) are integrated into a self-supporting porous carbon framework (PCF) to couple porous confinement with CPDs-mediated interfacial regulation. The resulting PCF-CPDs/I 2 -0.2 cathode substantially suppresses detectable accumulation of soluble polyiodide species, favors a predominantly direct I 2 /I − conversion pathway, facilitates interfacial charge transfer, improves iodine utilization, and enables long-term cycling stability in aqueous Zn–I 2 batteries.