Dynamic defects boost in-situ H₂O₂ piezocatalysis for water cleanup.

Abstract

Creating efficient catalysts for simultaneous H₂O₂ generation and pollutant degradation is vital. Piezocatalytic H₂O₂ synthesis offers a promising alternative to traditional methods but faces challenges like sacrificial reagents, harsh conditions, and low activity. In this study, we introduce a cobalt-loaded ZnO (CZO) piezocatalyst that efficiently generates H₂O₂ from H₂O and O₂ under ultrasonic (US) treatment in ambient aqueous conditions. The catalyst demonstrates exceptional performance with ~50.9% TOC removal of phenol and in situ generation of 1.3 mM H₂O₂, significantly outperforming pure ZnO. Notably, the CZO piezocatalyst maintains its H₂O₂ generation capability even after multiple cycles, showing continuous improvement (from 1.3 mM to 1.8 mM). This is attributed to the piezoelectric electrons promoting the generation of dynamic defects under US conditions, which in turn promotes the adsorption and activation of oxygen, thereby facilitating efficient H₂O₂ production, as confirmed by EPR spectrometry, XPS analysis, and DFT calculations. Moreover, the CZO piezocatalysts maintain outstanding performance in pollutant degradation and H₂O₂ production even after long periods of inactivity, and the deactivated catalyst due to metal ion dissolution could be rejuvenated by pH adjustment, offering a sustainable solution for wastewater purification.