Abstract

Urchin-like vanadium oxide nanostructures (VOx-NUs) were synthesized using V5+ alkoxide precursors [VO(OCH(CH3)2)3] and long-chain primary alkylamines (1-hexadecylamine and 1-octadecylamine) as structure-directing agents. The process involves intercalation-driven sol–gel assembly followed by hydrothermal treatment at 180 °C for seven days in aqueous–ethanolic media. The resulting spherical clusters are composed of densely packed, radially aligned vanadium oxide nanotubes stabilized by mixed-valence V4+/V5+ within a V7O162− lattice. Despite surface similarities to conventional VOx nanotubes, these urchin architectures exhibit distinct structural and electronic behavior due to their curved three-dimensional configuration and dense interfacial organization. Oxidation-state transitions were quantified via X-ray photoelectron spectroscopy (XPS) and volumetric titration, revealing progressive reduction of V5+ to V4+ templated by the amines. Magnetic characterization by SQUID magnetometry uncovered unusual room-temperature magnetic behavior, linked to the stabilization of mixed-valence states within the layered lattice. These results demonstrate how controlled intercalation and redox tuning enable the formation of VOx-NUs with emergent magnetic properties, expanding their potential in magnetoelectronic, catalytic, and sensing applications. The findings offer a novel framework for engineering multifunctional transition metal oxide nanostructures through oxidation-state modulation and self-assembly. © 2025 The Royal Society of Chemistry.