Abstract
Defect construction is a crucial approach to improve catalytic performance of peroxymonosulfate (PMS) activation, while elucidating the enhancement mechanism remains a great challenge. Herein, a metal-organic frameworks-derived, carbon-hybrid Mn2O3 with abundant oxygen vacancy (Mn2O3-NA-350) was synthesized and applied in a PMS-based advanced oxidation system for micropollutants degradation. Characterization and density functional theory calculation results show that the plentiful oxygen defects promote the formation of active Mn3+ species and the adsorption of PMS, which accelerate the electron shuttle and redox cycle of Mn3+/Mn4+ by enhancing electron donation of catalyst, and thus driving a 1O2-dominanted degradation pathway. As a result, the catalyst exhibits remarkable pollutant removal performance and structural durability, achieving over 95% degradation efficiency in 5min with an apparent reaction rate of 0.71min-1 ([2,4-dichlorophen] = 10mg/L, [catalyst] = 200mg/L, [PMS] = 200mg/L), and also maintaining almost unchanged catalytic performance after multiple cycles and even under a continuous flow operation for over 20hours. This work provided an effective Mn-based catalyst for PMS activation towards non-radical mediated pollutant elimination and revealed the oxygen vacancy-induced activity enhancement mechanism.
Published Version
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