Controllable synthesis of mesoporous multi-shelled ZnO microspheres as efficient photocatalysts for NO oxidation

Abstract

The successful application of hierarchically porous structure in environmental treatment has provided new insights for solving environmental problems. Hierarchically structured semiconductor materials were considered as promising photocatalysts for NO oxidation in gas phase. Multi-shelled ZnO microspheres (MMSZ) were controllably shaped with hierarchically porous structures via a facile hydrothermal route using amino acid (N-Acetyl-d-Proline) as template and post-calcination treatment. Symmetric Ostwald ripening was used to explain the morphological evolution of hierarchical nanostructure. MMSZ was proved highly efficient for oxidizing NO (400 ppb) in gas phase under UV light irradiation with a much higher photocatalytic removal rate (77.3%) than that of the as-obtained ZnO crystals with other hierachically porous structures, owing to its higher photocurrent intensity. Such greatly enhanced photocatalytic activity can be assigned to the enhanced crystallinity of ZnO, mesopores and unique multi-shelled structure. Enhanced crystallinity promotes photogenerated charges under light irradiation. Mesoporous porosity can ensure enough light scattering between the shells. Multi-shelled structure endows ZnO with higher specific surface area and high frequency of multiple light reflection, resulting in more exposed active sites, higher light utilization efficiency, and fast separation efficiency of photogenerated charge carriers. The experimental results demonstrated that the photogenerated holes (h+) are the main active species. Hierarchically structured ZnO is not only contributed to directly use solar energy to solving various problems caused by atmospheric pollution, but also has potential applications in energy converse and storage including solar cells, lithium batteries, water-splitting, etc.