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Easily Regenerated CuO/γ-Al<sub>2</sub>O<sub>3</sub> for Persulfate-Based Catalytic Oxidation: Insights into the Deactivation and Regeneration Mechanism

Jun Wang, Bin Li, Yang Li, Xiaobin Fan, Fengbao Zhang, Guoliang Zhang, Yuanzhi Zhu, Wenchao Peng

2021ACS Applied Materials & Interfaces56 citationsDOI

Abstract

In this work, γ-Al2O3-supported CuO (c-CuO/Al2O3) materials are successfully synthesized using a novel impregnation–precipitation–decomposition method. The obtained c-CuO/Al2O3 catalyst shows excellent catalytic activities for bisphenol A (BPA) degradation with sodium persulfate (PDS) as an oxidant. Radical quenching tests and electron paramagnetic resonance (EPR) studies indicate that PDS activation is a combined mechanism involving both free radical and nonfree radical pathways. In a continuous large-scale degradation process, about 1.78 L of 20 ppm BPA can be completely removed within 480 min. Although c-CuO/Al2O3 can be deactivated after several reaction cycles, the catalytic activity can be regenerated after simple aerobic calcination. X-ray photoelectron spectroscopy (XPS) and Raman analysis confirm that the deactivation of c-CuO/Al2O3 should be attributed to the conversion of Cu(II) to Cu(I). The aerobic calcination could oxidize Cu(I) back to Cu(II), thus recovering the catalytic activity. In addition, the density functional technology (DFT) and temperature-programmed oxidation (TPD) results reveal that γ-Al2O3 can not only serve as a carrier to anchor the CuO particles but also can adsorb and activate PDS by introducing more basic sites on the surface. c-CuO/Al2O3 has high activity and can be regenerated easily, thus having great potential applications for wastewater treatment.

Topics & Concepts

PersulfateCalcinationCatalysisX-ray photoelectron spectroscopyElectron paramagnetic resonanceMaterials scienceDecompositionAdsorptionInorganic chemistryDegradation (telecommunications)Catalytic oxidationPhotochemistryChemical engineeringPhysical chemistryChemistryOrganic chemistryNuclear magnetic resonanceTelecommunicationsEngineeringPhysicsComputer scienceAdvanced oxidation water treatmentAdvanced Photocatalysis TechniquesEnvironmental remediation with nanomaterials