Singlet-oxygen-driven Bisphenol A Degradation via Efficient Peroxymonosulfate Activation by MOF-derived Porous MnO-Mn6N2.58/N-C Catalysts

Nonradical oxidation via peroxymonosulfate (PMS) activation has attracted considerable attention for organic pollutant degradation, while the control and regulation of singlet oxygen ( 1 O 2 ) generation in catalytic oxidation are still challenging and the underlying mechanism remains ambiguous. In this paper, we synthesized a nitrogen-doped carbon-supported manganese-based catalyst by using ZIF-8 as a metal-organic framework (MOF) template for the in-situ loading of active components. When used for peroxymonosulfate activation, the MnO-Mn 6 N 2.58 /N-C catalyst exhibits a high Bisphenol A (BPA) degradation rate of 0.133   min -1 , exceeding PMS oxidation alone by 67 times. Mechanistic investigations reveal that the degradation process relies on the direct electron transfer from heterogeneous catalysts to PMS, contributing to efficient 1 O 2 generation for BPA degradation via a nonradical pathway. We demonstrate that Mn(II)/Mn(III) redox cycling on the catalyst surface activates PMS into superoxide (O 2 • - ), which in turn converts into 1 O 2 , thereby elucidating the underlying mechanism for high-efficiency degradation. This work provides a novel strategy to design heterogeneous Mn-based catalysts for recalcitrant organic wastewater remediation via a nonradical oxidation pathway.