Graduate Thesis Or Dissertation

 

The Role of Materials Chemistry in Designing Advanced Color Inorganic Pigments 公开 Deposited

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  • The results of the research presented in this work are related to synthesis and investigations of novel color inorganic pigments having various structures and shades. Inorganic pigments play a major role in contemporary life. They are used in paints, rubber, plastic, cosmetics etc. Searching for new, stable, environmentally benign and cheap pigments is an important task of materials science. Several classes of colored inorganic oxides have been prepared and studied using various methods and techniques including powder X-ray (XRD) and neutron diffraction, color characterization (L*a*b* parameters), optical (UV-VIS diffuse reflectance and near-IR (NIR) reflectance), magnetic and dielectric properties measurements, infrared (IR) spectroscopy. Pigments A₅Mʹ₃₋ₓMₓO₁₂X (A = Sr, Ba; Mʹ = Cr, Mn; M = V, P; X = F, Cl) with apatite-type structure were prepared using standard solid state, sol-gel and microwave synthesis methods. All samples have bright colors varying from white (x = 3.0) through turquoise (x = 1.5) to dark green (x = 0). The color arises due to a combination of d-d interatomic transitions of Mn⁵⁺/Cr⁵⁺ cations and transition metal–O²⁻ charge transfer. Mn⁵⁺, V⁵⁺ and P⁵⁺ occupy the tetrahedral sites in the structure as shown by Rietveld structure refinement of neutron data. Hibonite – type colored oxides with a general formula of AAl₁₂₋ₓMₓO₁₉ (A = Ca, Sr, RE (rare earths) or any combination thereof; M = Ni, Fe, Mn, Cr, Cu coupled with one of the following: Ga, In, Ti, Sn, Ge, Nb, Ta, Sb) were synthesized through A-site and M-site substitutions. Ni, Fe, Mn, Cr and Cu are chromophore ions and they are responsible for the color of the compounds. Ni²⁺ gives bright sky-blue to royal-blue colors; samples containing different amounts of Fe, Mn, Cr or Cu have diverse colors: ivory, brown, creamy, tan, pink, light turquoise and green. Ni²⁺, Mn²⁺ and Fe³⁺ prefer to occupy the tetrahedral site, Mn³⁺ has a preference for both tetrahedral and octahedral sites, Ti⁴⁺ and Sn⁴⁺ for octahedral site in the hibonite structure. Compounds belong to Li₂Mn₁₋ₓTiₓO₃ (x = 0–1.0) series show bright orange colors varying from dark brick red (x = 0) to orange (x = 0.5) and light orange (x = 0.8). d-d transitions of d electrons of octahedral Mn⁴⁺ and M(IV)–O²⁻ charge transfer are responsible for the colors. Pigments with sillenite-type structure, Bi₁₂₋ₓInₓTiO₂₀ (x = 0–1.5), Bi₁₂₋ₓInₓMn₀.₂Ti₀.₈O₂₀ (x = 0–5.5) and Bi₁₂Mn₁₋ₓMxO₂₀ (M = Ti, Si, Ge), were prepared using standard solid state synthesis through Bi-site and M-site substitutions. Bi₁₂-ₓInₓTiO₂₀ compounds have shades changing from light yellow (x = 0) to beige (x = 1.5); Bi₁₂-ₓInₓMn₀.₂Ti₀.₈O₂₀ series: from forest green (x = 0) to dark sea green (x = 2.5) and light olive drab (x = 5.5); Bi₁₂Mn₁₋ₓMₓO₂₀ (M = Ti, Si, Ge): from dark green (x = 0) to forest green (x = 0.5) and lawn green (x = 0.8); Bi₁₂MO₂₀ (M = Ti, Si, Ge) are light yellow. Mn⁴⁺ (Td) is a chromophore element of the solid solutions, samples become lighter when amount of manganese decreases. Bi₁₂Mn₁₋ₓTiₓO₂₀ (x = 0.2; 0.6; 0.8) phases show paramagnetic behavior in the measured temperature region (5–300 K). All synthesized samples have relatively high reflectance in the near-IR region (700–2500 nm) and are promising candidates for “Cool pigments” applications.
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