<p>Metal-oxide functionalized carbon nanotube (CNT) nanocomposites (Ce<sub>2</sub>O<sub>3</sub>@A-MWCNTs and Nb<sub>2</sub>O<sub>5</sub>@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<sup>⋅</sup>) and superoxide radical (O<sub>2</sub><sup>−</sup>) 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<sup>−1</sup>; 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<sup>−1</sup> (Nb<sub>2</sub>O<sub>5</sub>@A-MWCNTs) and 0.037 ± 0.008 min<sup>−1</sup> (Ce<sub>2</sub>O<sub>3</sub>@A-MWCNTs), which indicates an efficient interfacial charge transfer at the inorganic junction (CNTs-oxide). The catalysts also showed excellent usability with &gt; 85–88% degradation efficiency after 10 cycles at 200 ppm, indicating stability for the repeated use of solar energy for wastewater remediation.</p>

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Band-Gap Engineering at Rare-Earth Metal Oxide–Carbon Nanotubes Interfaces: Sunlight Photocatalysis of Methylene Blue and Crystal Violet Under Highly Concentrated Conditions

  • Sultan Muhammad,
  • Naseem Bano,
  • Ammara Aftab,
  • Taiba Naseem,
  • Shams ur Rahman,
  • Muhammad Waseem

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.