Facilitating reactive oxygen species (ROS) generation is an effective way to promote the heterogeneous catalytic efficiency for organics removal. However, the metal leaching in metal-based catalysts and the low activity of non-metallic materials restrict ROS production. In this work, the purpose was achieved by loading a small amount of spinel CuFeO onto porous carbon nitride substrate. The synthesized CuFeO@O-CN composite first to activate peroxymonosulfate (PMS), which produce a plenty of ROS (•OH, SO• and O) for organics removal, leading to highly oxidation for diverse organics. Through the comparative analysis of the surface composition before and after reaction, we found that the interface multi-electron transfer routs, including surface Cu(II)/Cu(I), Fe(III)/Fe(II) and their cross interaction, participated in the redox cycle, giving rise to the rapid and massive production of ROS, so that DMPO and TEMP were instantly oxidized in electron paramagnetic resonance (ESR) detection. Importantly, the carrier of porous O-CN, which acted as the electron transfer mediator, not only favors PMS adsorption via surface -OH, but also facilitates the conversion between different metal species. As a result, the CuFeO@O-CN/PMS system can remove 99.1% BPA and achieve 52.6% mineralization under optimized conditions. Thus, this study not only sheds light on the tailored design of heterogeneous catalyst for organics removal and elucidates the interfacial catalytic mechanisms for PMS activation.

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http://dx.doi.org/10.1016/j.chemosphere.2022.134511DOI Listing

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