Oxygen Vacancies in Piezoelectric ZnO Twin-Mesocrystal to Improve Peroxymonosulfate Utilization Efficiency via Piezo-Activation for Antibiotic Ornidazole Removal.

ABSTRACT

Piezoelectric mesocrystals as defective materials have been demonstrated to possess adsorptive and catalytic properties in redox reactions. However, there is still a lack of research on the quantitative relationship between the defect concentration and the piezocatalytic performance in piezoelectric mesocrystals. Herein, twin-hierarchical structure ZnO piezoelectric mesocrystals are taken with different oxygen-vacancies (OVs) concentrations to quantitatively investigate the effect of defect content on the peroxymonosulfate (PMS) piezo-activation in water purification. The ZnO piezoelectric mesocrystal with moderate OVs concentration exhibits a rapid antibiotic ornidazole (ORZ) pollutants degradation rate (0.034 min-1 ) and achieves a high PMS utilization efficiency (0.162) that exceeds the most state-of-the-art catalytic processes, while excessive OVs suppressed the piezocatalytic performance. Through calculations of electron property and reactants affinity, a quantitative relationship between OVs concentration and piezocatalytic properties is established. The ZnO mesocrystal with moderate OVs concentration realized increased electron delocalization, reduced charge transfer barrier, and enhanced reactants affinity, thus accelerating the kinetics of PMS activation. This work provides theoretical guidance for the application of defect engineering in mesocrystal to realize enhanced piezocatalytic performance.