Interfacial Charge Redistribution-Driven Two-Electron Conversion in Ni_0.85Se@Mo-Doped NiCo-LDH for High-Power...

Rational structural engineering and electronic modulation are vital for advancing high-performance electrochemical energy storage. Herein, we construct a hierarchical Ni_0.85Se@Mo-doped NiCo-LDH heterostructure (NS@MNC-LDH) directly on hydrophilic carbon cloth (HCC) to achieve uniform nucleation and strong interfacial coupling (NS@MNC-LDH/HCC). The conductive Ni_0.85Se core provides fast electron transport and mechanical robustness, while the Mo-doped NiCo-LDH shell introduces abundant oxygen vacancies and optimized electronic states to enrich redox-active sites. Combined experiments and density functional theory calculations reveal pronounced interfacial charge redistribution that accelerates ion/electron transport and enables efficient multi-electron transfer. Distribution of relaxation times analysis and in situ Raman spectroscopy further verify rapid charge-transfer kinetics and highly reversible NiCo-LDH/Ni(Co)OOH/Ni(Co)O₂ conversions. Benefiting from these synergistic effects, NS@MNC-LDH/HCC delivers an ultrahigh capacity of 540.8 mAh g^-1 at 1 A g^-1, approaching a two-electron transfer capacity, along with 81.8% retention at 32 A g^-1. The assembled hybrid supercapacitor achieves an energy density of 128.5 Wh kg^-1 at 750 W kg^-1 and maintains 83.8% of its capacity after 10 000 cycles. This work demonstrates that interfacial electronic coupling combined with defect-regulated multi-electron transfer provides a powerful and generalizable design principle for next-generation high-power energy storage materials.