Surface defect engineering is a promising strategy for enhancing the number of surface-active sites to facilitate efficient redox reactions that occur on the surface of a photocatalyst. A green approach was employed to prepare urea- and choline-chloride-based deep eutectic solvent (DES) for the synthesis of ZnO/Zn(OH)2 supported by a DES complex (Zn precursor). Surface defects on ZnO nanoparticles (NPs) were tailored by decomposing the Zn precursor in air. In addition, calcination improved the crystallinity and surface-active sites of the defective ZnO by creating surface oxygen vacancies (Vo). The appearance of an Electron paramagnetic resonance peak at a g value of 1.96 confirms the formation of single-charged Vo defects on the surface of ZnO. The photocatalyst prepared at a reaction bath temperature of 75 °C (Vo-ZnO-75) showed the highest photocatalytic activity. The observed green emission in the photoluminescence spectrum and X-ray photoelectron spectroscopy analysis suggests the formation of defects on the ZnO surface. Consequently, Vo-ZnO-75 enhanced surface donor density (14.4×1020 cm−3) and lower charge transfer resistance (88.89 × 103 Ω). The optimized photocatalyst of Vo-ZnO-75 has 94% removal efficiency for rhodamine B degradation within 60 min. This study sheds new light on the development of an efficient and eco-friendly approach for preparing defective ZnO NPs for photocatalytic applications.
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