Photocatalytic desulfurization of crude oil under visible light using N-doped TiO2 nanoparticles
摘要
Nitrogen-doped TiO2 (N-TiO2) nanoparticles were synthesized by a green co-precipitation method using Taraxacum officinale (dandelion) flower extract as a natural capping agent and urea as the nitrogen source. The synthesized materials were characterized by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), field-emission scanning electron microscopy/energy-dispersive spectroscopy (FE-SEM/EDS), X-ray photoelectron spectroscopy (XPS), UV–Vis diffuse reflectance spectroscopy (DRS), and BET surface area analysis. N-doped TiO2 exhibited a pure anatase phase with a crystallite size of 10.08 nm, a BET surface area of 92.7 m2/g, and a reduced optical band gap of 2.78 eV, compared to 56.3 m2/g and 3.20 eV for undoped TiO2. Under optimized conditions (120 mg catalyst, 2.0 mL H2O2, 10.0 mL acetonitrile, 800 rpm, 90 min, 298 K), N-doped TiO2 removed 63.5 ± 1.2% of the sulfur from real crude oil (initial sulfur content 3.527 wt.%) under 50 W visible-light LED irradiation, compared to 30.2 ± 0.9% for undoped TiO2 and 1.0% for a no-catalyst control. Under UV irradiation, N-doped TiO2 achieved 56.7 ± 1.0% removal versus 46.3 ± 0.8% for undoped TiO2. Radical scavenger experiments confirmed that both hydroxyl radicals (·OH) and superoxide anion radicals (O2·⁻) contribute to desulfurization. The catalyst retained above 55% efficiency after five consecutive reuse cycles. These results demonstrate that a simple and inexpensive green synthesis route can produce a visible-light-active N-doped TiO2 photocatalyst effective for direct crude oil desulfurization under mild conditions.