Rare-Earth-Induced Structural Modulation of NiFe₂O₄ for High-Energy Asymmetric Supercapacitor Devices

The rational design of electrode materials with tailored composition and architecture is crucial for advancing high-capability electrochemical energy storage systems. This study reports that gadolinium-modified NiFe₂O₄ nanosheet electrodes were effectively synthesized on nickel foam via a hydrothermal approach followed by thermal treatment. A series of compositions (NiFe, NiFe–Gd1, NiFe–Gd2, and NiFe–Gd3) were prepared to systematically examine the effect of Gd incorporation on structural features and electrochemical properties. X-ray diffraction (XRD) analysis confirmed the formation of the cubic spinel NiFe₂O₄ phase without detectable secondary phases, indicating that the crystal structure remains intact after Gd introduction. X-ray photoelectron spectroscopy (XPS) further verified the presence of Ni²⁺, Fe³⁺, and Gd³⁺ species within the lattice environment. Morphological analysis using field-emission scanning electron microscopy (FESEM) revealed a nanosheet-based architecture, where the optimized NiFe–Gd2 electrode exhibited a porous and interconnected nanosheet framework with abundant exposed edges. This structural configuration improves electrolyte penetration and facilitates efficient ion transport during charge storage processes. Electrochemical measurements demonstrated that the NiFe–Gd2 electrode delivers an areal capacitance of 5235 mF cm⁻² at 10 mA cm⁻², along with improved reaction kinetics and low internal resistance. An asymmetric supercapacitor assembled using NiFe–Gd2 as the positive electrode and activated carbon as the negative electrode operated stably within a 0–1.5 V potential window, achieving an energy density of 0.136 mWh cm⁻² and a power density of 3.14 mW cm⁻², while retaining 86.55% of its initial capacitance after 7000 cycles. These results highlight the potential of rare-earth engineering as a viable strategy for designing advanced spinel ferrite electrodes and pave the way for the development of high-performance, durable, and scalable supercapacitor systems for practical energy storage applications.