Tunable Surface Charge Redistribution via Lattice Strain Engineering in B/Mo Co‐Doped NiV 2 O 6 for High‐Power Supercapacitors

Abstract The pursuit of high‐energy‐density supercapacitors remains challenged by the irreversible surface charge accumulation and sluggish ion dynamics in conventional vanadate cathodes. To address these limitations, a lattice strain engineering strategy is devised through B/Mo co‐doping in NiV 2 O 6 , which enables dynamic regulation of surface charge distribution via atomic‐level stress manipulation. Density functional theory (DFT) calculations demonstrate that high‐valence Mo 6+ induces compressive lattice strain (–4.4%) to strengthen metal‐oxygen covalency, while low‐electronegativity B 3+ generates tensile strain (+ 2.9%) that enhances surface hydroxyl affinity. This strain dichotomy optimizes OH − adsorption energetics by 0.28 eV and creates gradient oxygen vacancy. The cooperative dopant effects significantly enhance charge‐transfer kinetics, endowing the B/Mo‐NiV 2 O 6 /NF electrode with a superior specific capacitance of 2850 F g −1 (1 140 C g −1 ) at 1 A g −1 . In situ Raman reveals reversible oxygen vacancy migration along (004) crystallographic planes during cycling, which dynamically dissipates structural stress. A solid‐state asymmetric supercapacitor delivers a 1.8 V operational window with remarkable energy/power density (38.35 Wh kg −1 /900 W kg −1 ) and 75% capacity retention after 10 000 cycles. Practical viability is demonstrated by powering 20 parallel‐connected light‐emitting diodes (LEDs). This work pioneers a lattice strain‐mediated surface charge regulation paradigm for durable high‐power energy storage.