Uzair Ahmed Kolachi, Rajapriya Andavar, Anuj Kumar, Yi He, Ali Raza, Yanzhi Sun, Junqing Pan
The electrode-electrolyte interface engineering is paramount to advancing bifunctional porous carbon materials for zinc-hybrid supercapacitors (ZHSCs) and sodium-ion batteries (SIBs). Herein, a coordination-pyrolysis method is proposed to synthesize Ag-nanoparticle-decorated bimetallic MOF-derived carbon nanorods (Ag-BMNR-2), wherein the interfacial architecture is synergistically engineered through three mechanisms: (i) evenly dispersed Ag nanoparticles introduce electron-rich colloidal sites that reduce charge-transfer resistance and accelerate interfacial electron transport via a continuous Ag → Ag → Ag conductive network; (ii) chemical activation generates oxygen-rich surface functionalities (CO, CO, OH) that enhance electrolyte wettability and provide dipole-ion coupling sites for Na+ coordination; and (iii) a hierarchical micro-mesoporous architecture maximizes ion-accessible interfacial area. Theoretical calculations and in/ex situ characterization confirm that Ag doping lowers the Na+ diffusion barrier, strengthens adsorption affinity, and elevates the electronic density of states near the Fermi level. Benefiting from this synergistically engineered interface, Ag-BMNR-2 delivers 364.7 F g-1 at 1 A g-1, retaining 95.6% capacity after 100,000 cycles in SCs, and achieves 458.6 mAh g-1 at 0.05 A g-1 with 90.1% capacity retention over 700 cycles in SIBs (ICE: 69.9%). This work establishes interface engineering of Ag-decorated hierarchical porous carbon as a versatile strategy for dual-functional energy storage materials.