ABSTRACT
Plasmonic-enhanced photocatalysis using visible light is considered a promising strategy for pollution photodegradation. However, there is still a lack of comprehensive and quantitative understanding of the underlying mechanisms and interactions involved. In this study, we employed a two-step process to fabricate arrays of ZnO nanosheets decorated with Au nanoparticles (Au-ZnO NS). Various characterization techniques were used to examine the morphological, structural, and chemical properties of the fabricated Au-ZnO NS array. Furthermore, we systematically investigated the photocatalytic degradation of methyl orange under visible light irradiation using Au-ZnO NS arrays prepared with varying numbers of photochemical reduction cycles. The results indicated that as the number of photochemical reduction cycles increased, the photodegradation efficiency initially increased but subsequently decreased. Under visible light irradiation, the Au-ZnO NS array obtained via four cycles of photochemical reduction exhibits the highest photocatalytic degradation rate of methyl orange 0.00926 min-1, which is six times higher than that of the ZnO NS array. To gain a better understanding of the plasmonic effect on photodegradation performance, we utilized electromagnetic simulations to quantitatively investigate the enhancement of electric fields in the Au-ZnO NS array. The simulations clearly presented the nonlinear dependencies of electric field intensity on the distribution of Au nanoparticles and the wavelength of radiation light, leading to a nonlinear enhancement of hot electron injection and eventual plasmonic photodegradation. The simulated model, corresponding to four cycles of photochemical reduction, exhibits the highest electric field intensity at 550 nm, which can be attributed to its strong plasmonic effect. This work provides mechanistic insights into plasmonic photocatalysts for utilizing visible light and represents a promising strategy for the rational design of high-performance visible light photocatalysts.
ABSTRACT
Supported nanostructured photocatalysis is considered to be a sustainable and promising method for water pollution photodegradation applications due to its fascinating features, including a high surface area, stability against aggregation, and easy handling and recovery. However, the preparation and morphological control of the supported nanostructured photocatalyst remains a challenge. Herein, a one-step hydrothermal method is proposed to fabricate the supported vertically aligned ZnO nanosheet arrays based on aluminum foil. The morphologically controlled growth of the supported ZnO nanosheet arrays on a large scale was achieved, and the effects of hydrothermal temperature on morphologic, structural, optical, and photocatalytic properties were observed. The results reveal that the surface area and thickness of the nanosheet increase simultaneously with the increase in the hydrothermal temperature. The increase in the surface area enhances the photocatalytic activity by providing more active sites, while the increase in the thickness reduces the charge transfer and thus decreases the photocatalytic activity. The influence competition between the area increasing and thickness increasing of the ZnO nanosheet results in the nonlinear dependence between photocatalytic activity and hydrothermal temperature. By optimizing the hydrothermal growth temperature, as fabricated and supported ZnO nanosheet arrays grown at 110 °C have struck a balance between the increase in surface area and thickness, it exhibits efficient photodegradation, facile fabrication, high recyclability, and improved durability. The RhB photodegradation efficiency of optimized and grown ZnO nanosheet arrays increased by more than four times that of the unoptimized structure. With 10 cm2 of as-fabricated ZnO nanosheet arrays, the degradation ratio of 10 mg/L MO, MB, OFL, and NOR was 85%, 51%, 58%, and 71% under UV irradiation (365 nm, 20 mW/cm2) for 60 min. All the target pollutant solutions were almost completely degraded under UV irradiation for 180 min. This work offers a facile way for the fabrication and morphological control of the supported nanostructured photocatalyst with excellent photodegradation properties and has significant implications in the practical application of the supported nanostructured photocatalyst for water pollution photodegradation.
