Enhanced Al³⁺ storage performance of NiSe₂@N, S co-doped carbon sphere cathodes for aqueous aluminum-ion batteries
摘要
Aqueous aluminum-ion batteries are limited by sluggish Al³⁺ diffusion kinetics, structural instability, and rapid capacity degradation caused by passivation reactions in aqueous electrolytes. To address these challenges, a NiSe₂-decorated porous nitrogen and sulfur co-doped carbon sphere composite (NiSe₂@PNSCS, NSPNSCS) was developed as a cathode material. The composite was synthesized through two-step hydrothermal process by chemical activation, and its structural, morphological, and electrochemical characteristics were investigated using XRD, SEM, XPS, galvanostatic charge–discharge, electrochemical impedance spectroscopy, ex-situ evaluation, and cyclic voltammetry. NSPNSCS cathode delivered a reversible capacity of 60 mAh g⁻¹ at 200 mA g⁻¹, exhibited discharge capacities ranging from 82 to 25 mAh g⁻¹ as current density increased from 200 to 600 mA g⁻¹, and maintained ~ 98% capacity retention with coulombic efficiency above 90% over 1000 cycles at 500 mA g⁻¹. The Al³⁺ diffusion coefficients were calculated as 6.499 × 10⁻¹⁷ cm² s⁻¹ for the fresh cell and 1.062 × 10⁻¹⁷ cm² s⁻¹ after cycling, while ex-situ XRD confirmed reversible lattice contraction of up to 2.1%, indicating elastic structural behavior during Al³⁺ intercalation. These results shows that NSPNSCS were promising cathode material for cost-effective, high-stability aqueous aluminum-ion batteries suitable for renewable energy and large-scale energy storage uses.