Realizing One-Step Two-Electron Transfer of Naphthalene Diimides Via a Regional Charge Buffering Strategy for Aqueous Organic Redox Flow Batteries.

Naphthalene diimide derivatives show great potential for application in neutral aqueous organic redox flow batteries (AORFBs) due to their highly conjugated molecular structure and stable two-electron storage capacity. However, the two-electron redox process of naphthalene diimides typically occurs via two separate steps with the transfer of one electron per step ("two-step two-electron" transfer process), which leads to an inevitable loss of voltage and energy. Herein, we report a novel regional charge buffering strategy that utilizes the core-substituted electron-donating group to adjust the redox properties of naphthalene diimides, realizing two electron transfer via a single-step redox process ("one-step two-electron" transfer process). The symmetrical battery testing of NDI-DEtOH revealed exceptional intrinsic stability lasting for 11 days with a daily decay rate of only 0.11%. Meanwhile, AORFBs with NDI-DMe/FcNCl and NDI-DEtOH/FcNCl exhibited a remarkable 40% improvement in peak power density at 50% state of charge (SOC) in comparison to NDI/FcNCl-based AORFBs. In addition, the battery's energy efficiency has increased by 24%, resulting in much more stable output power and significantly improved energy efficiency. These results are of great significance to practical applications of AORFBs.