Comparative Structural, Phase Evolution, and Spectroscopic Investigation of Binary and Ternary Mixed Metal Oxide Nanoparticles (Co-Cu, Co-Ni, Ni-Fe, And Co-Ni-Zn) Synthesized Via Grape Leaf Powder Calcination

Mixed transition metal oxide nanostructures have attracted a lot of interest in science and technology because they show electronic, catalytic and magnetic behavior than single-metal oxides. In this study we compare four mixed metal oxide systems made using a green method. The samples are: ternary Co-Ni-Zn (Sample 1) binary Co-Cu (Sample 2) binary Co-Ni (Sample 3) and binary Ni-Fe (Sample 4). All of them were made using grape leaf powder from waste (Vitis vinifera) as a natural material to help form the structure reduce metal ions and shape the nanostructures. After that the materials were heated at 500°C to get the product. We looked at the structure crystal phases, particle size, chemical bonds and surface purity using X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FTIR). The XRD results showed that the way the metal ions fit into the crystal lattice depends on their size how strongly they attract electrons and how their d-electrons arrange. In the Co-Cu and Co-Ni-Zn systems the different metal ions didn’t mix well leading to phases: Co₃O₄ with CuO and Co₃O₄ with NiO and ZnO. This happened because of Jahn-Teller distortion and the tendency of the ions to separate. In the Co-Ni system, a slight XRD peak shift to 37.2° suggests the possible formation of a Co-Ni solid solution (CoNiO₂); however, this assignment remains tentative and requires quantitative phase analysis such as Rietveld refinement for confirmation.The Ni-Fe system showed reflections consistent with inverse spinel NiFe₂O₄ along with NiO and α-Fe₂O₃; quantitative phase refinement would be needed to establish the relative phase fractions and degree of spinel formation. The average size of the particles was between 50 and 70 nanometers and this was controlled by how the metal ions moved and how crystals grew. The Ni-Fe sample had a peak at 668 cm⁻¹, which is typical for spinel ferrites showing both tetrahedral and octahedral bonding. Interestingly the materials with nickel helped burn off carbon effectively leaving very little leftover organic material. This was not the case, for the copper- or zinc-based samples. Residual carbon-oxygen bonds (1045 cm⁻¹) and surface hydroxyl groups (3394–3423 cm⁻¹) were still present which means the biocapping process was stable and eco-friendly. Because of these features these materials could be used in cleanup, photocatalysis and magnetic treatment applications.

Green synthesis, Mixed metal oxides, Grape leaf powder, Phase evolution

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