Integrated Theoretical and Experimental Investigation of the Fe<sub>12</sub>B<sub>2</sub>N<sub>2</sub>Phase as a Potential Electrode Material for Energy Storage
CHEMISTRY OF MATERIALS, 2026 (SCI-Expanded, Scopus)
- Yayın Türü: Makale / Tam Makale
- Basım Tarihi: 2026
- Doi Numarası: 10.1021/acs.chemmater.6c02322
- Dergi Adı: CHEMISTRY OF MATERIALS
- Derginin Tarandığı İndeksler: Science Citation Index Expanded (SCI-EXPANDED), Scopus, Chemical Abstracts Core, Chimica, Compendex, INSPEC
- Kocaeli Üniversitesi Adresli: Evet
Özet
Transition metal-boron-nitrogen ternary compounds have significant potential for electrochemical energy storage, yet their structure-property relationships are not fully understood. This study investigates the synergistic effects of integrating iron, boron, and nitrogen within a single ternary phase through a mechanical activation-assisted synthesis route. Using melamine (C3H6N6) as the nitrogen source, the effects of mechanical activation, molar ratio, and annealing temperature on phase evolution were systematically examined, revealing the sequential formation of FeB and Fe-rich Fe3B/Fe3N intermediate phases prior to the formation of the Fe12B2N2 phase. First-principles calculations confirmed the dynamical stability and metallic character of the ternary phase through phonon dispersion and electronic band structure analyses. Structural characterization by X-ray diffraction (XRD), Raman spectroscopy, and high-resolution transmission electron microscopy (HR-TEM) showed good agreement with the first-principles calculations, supporting the structural assignment of the orthorhombic Fe12B2N2 phase. The electrochemical performance of the synthesized powders was evaluated as supercapacitor electrode materials, revealing that the sample exhibiting the most well-defined Fe12B2N2 phase, together with the smallest particle size (79.4 nm), delivered a specific capacitance of 6.77 F/g and an energy density of 2.17 Wh/kg. Furthermore, the electrodes exhibited high power densities ranging from 41.4 to 70.2 kW/kg, demonstrating rapid charge-discharge capability while maintaining Coulombic efficiencies above 98% over 5000 charge-discharge cycles. Electronic structure analysis revealed that the simultaneous incorporation of B and N increases the Fe d-state density near the Fermi level relative to the corresponding binary compounds, providing a microscopic explanation for the improved electrochemical performance of the ternary phase. These findings suggest that Fe12B2N2-based nanocompounds are promising electrode materials for high-power and durable electrochemical energy storage.