RESUMO
Sulfur compounds in fuel such as thiophene, benzothiophene and dibenzothiophene are the primary source of SO x emissions, leading to environmental pollution and acid rain. In this study, we synthesized a layered oxygen-doped graphitic carbon nitride (OCN) structure and integrated ZnO and TiO2 nanoparticles onto the OCN surface through a microwave-assisted sol-gel method. The X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) results confirmed a robust interaction between the ZnO and TiO2 nanoparticles and the oxygen-doped g-C3N4 (OCN) surface, as indicated by the formation of C-N-Ti and C-O-Ti bonds. This interaction notably improved the optoelectronic properties of the ZnO-TiO2/OCN composite, yielding increased visible light absorption, reduced charge recombination rate, and enhanced separation and transfer of photogenerated electron-hole pairs. The oxygen doping into the CN network could alter the band structure and expand the absorption range of visible light. The ZnO-TiO2/OCN photocatalyst demonstrated remarkable desulfurization capabilities, converting 99.19% of dibenzothiophene (DBT) to dibenzothiophene sulfone (DBT-O2) at 25 °C, and eliminating 92.13% of DBT from real-world fuel oil samples. We conducted in-depth analysis of the factors impacting the redox process of DBT, including the ZnO ratio, initial DBT concentration, catalyst dosage, stability, and O/S molar ratio. Radical trapping experiments established that ËO2 -, ËOH and h+ radicals significantly influence the reaction rate. The obtained results indicated that the ZnO-TiO2/OCN photocatalyst represents a promising tool for future fuel oil desulfurization applications.
RESUMO
This study delves into the advanced integration of a ternary heterogeneous Z-scheme photocatalyst, TiO2/CuInS2/OCN (OCN: O-g-C3N4), with carbon quantum dot (CQD) to improve the degradation efficiency of reactive yellow 145 (RY145) dye in water. Through a systematic examination, we elucidated the photocatalytic mechanisms and the role of radicals, electrons, and holes in the treatment process. Our findings revealed that this novel catalyst integration significantly boosted RY145 degradation efficiency, achieving 98.2%, which is markedly higher than the efficiencies which could be achieved using TiO2/CuInS2/OCN alone. Moreover, the TiO2/CuInS2/OCN/CQD photocatalyst demonstrated superior rate performance over its components. Comprehensive evaluations, including photoelectrochemical and radical tests, further confirmed the efficiency of the integrated system, adhering to Z-scheme principles. The catalyst showcased remarkable stability, with over 94% reusability after five reaction cycles. These findings pave the way for the potential use of the TiO2/CuInS2/OCN/CQD photocatalyst as an innovative solution for water pollutant treatment via photocatalytic technology.
RESUMO
Semiconductor-containing porous materials with a well-defined structure could be unique scaffolds for carrying out selective organic transformations driven by visible light. We herein introduce for the first time a heterostructure of silver indium sulfide (AgInS2) ternary chalcogenide and a highly porous MIL-101(Cr) metal-organic framework (MOF) synthesised from polyethylene terephthalate plastic waste. Our results demonstrate that AgInS2 nanoparticles were uniformly attached to each lattice plane of the octahedral MIL-101(Cr) structure, resulting in a nanocomposite with a high distribution of semiconductors in a porous media. We also demonstrate that the nanocomposite with up to 40% of AgInS2 doping exhibited excellent catalytic activity for tetracycline degradation under visible light irradiation (â¼99% tetracycline degraded after 4 h) and predominantly maintained its performance after five cycles. These results could promote a new material circularity pathway to develop new semiconductors that can be used to protect water from further pollution.