Precision Synthesis and Modulation of Ion Diffusion Interface.

The development of electrochemical energy storage systems with high-density storage sites is the key and core technology to achieve transformative breakthroughs in battery performance. Herein, we immobilize redox-active naphthalene diamides (TBNDI) within 2D graphdiyne (GDY) to construct carbon-based TBNDI-GDY composite electrodes. This approach creates a hierarchical ion diffusion pathway and enables tunable electronic modulation through a strategic molecular design. The multiredox center electrodes demonstrate prominent kinetic processes, superior interfacial compatibility, and fast desolvation capability. The as-prepared electrodes with pseudocapacitive processes display ultrahigh specific capacity up to 2079 mAh/g at 0.1 A/g, remarkable rate capacity, and ultralong stability for 10,000 cycles even at 5 A/g. Dynamic kinetic tracking and lithium active site visualization confirm that capacity contribution originates from reversible lithium-ion capture as well as Li-C orbital coupling in the sloping voltage regions, nanopore filling, and graphitic region interaction in the subsequent voltage region. Moreover, C=O-N groups with lone pair electron delocalization could modulate the electronic structure and promote reversible redox activities. Our findings highlight that the rational design of the ion diffusion interface from the basic chemical structure can provide giant evolution on the properties of the electrode material for high performance batteries.