Band-Gap Engineering at Rare-Earth Metal Oxide–Carbon Nanotubes Interfaces: Sunlight Photocatalysis of Methylene Blue and Crystal Violet Under Highly Concentrated Conditions
摘要
Metal-oxide functionalized carbon nanotube (CNT) nanocomposites (Ce2O3@A-MWCNTs and Nb2O5@A-MWCNTs) were prepared by the hydrothermal technique and analyzed as sunlight-active photocatalysts for degradation of methylene blue (MB) and crystal violet (CV). The combination of a CNT conductive network (for increased electron transport and charge separation properties) and redox active oxide domains (for reactive oxygen species formation, such as production of hydroxyl radicals (OH⋅) and superoxide radical (O2−) in the hybrid architecture inhibits electron–hole recombination and promotes substantial dye mineralization at the oxide-CNT interface through improved interfacial charge transfer and reactive oxygen species generation. In the presence of direct sunlight (UV index 8–10) and alkaline environment (pH 8–10), degradation of CV (76.75–79.13%) and degradation of MB (90.83–93.32%) were achieved. With prolonged irradiation time to 240 min, near complete removal was obtained, with MB degradation of 97.98–99.61% and CV degradation of 98.74–99.81%. On the other hand, Increasing the initial dye concentration decreased photocatalytic performance (up to 200 mg L−1; 83.78–92.09%), in accordance with light-screening effects with the adsorption of reaction intermediates. Moreover, kinetic analysis was used to corroborate heterogeneous, surface-controlled behavior, for which the rate constant for CV was of the pseudo-first order 0.023 ± 0.003 min−1 (Nb2O5@A-MWCNTs) and 0.037 ± 0.008 min−1 (Ce2O3@A-MWCNTs), which indicates an efficient interfacial charge transfer at the inorganic junction (CNTs-oxide). The catalysts also showed excellent usability with > 85–88% degradation efficiency after 10 cycles at 200 ppm, indicating stability for the repeated use of solar energy for wastewater remediation.