Abstract
For improving the catalytic activity and recyclability of CuS in Fenton-like reaction processes, novel sulfur vacancies-enriched CuS@MIL-101(Fe) was constructed, characterized, and examined as heterogeneous catalysts for activating peroxymonosulfate (PMS) to degrade coumarin (COU). Thanks to the redox pairs of Fe3+/Fe2+, Cu+/Cu2+, S2−/S22−/S0/sulfate species, copper-iron synergistic effect and sulfur vacancies, the CuS@MIL-101(Fe) realized a complete removal of COU (30 μM) in 10 min with reaction rate constant of 0.577 min−1, which was 11.1 and 17.0 times of CuS and MIL-101(Fe), respectively. The effect of various experimental conditions (i.e., initial pH, CuS@MIL-101(Fe) dosage, PMS concentration, and background anions) on COU degradation was discussed, and the stability and versatility of CuS@MIL-101(Fe) was studied as well. Radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy identified •OH and 1O2 as the main reactive oxygen species (ROS). Finally, the possible mechanism of higher COU degradation efficiency in the CuS@MIL-101(Fe) activated PMS system and the degradation pathways were also deeply explored. Consequently, this work provided a novel insight into construction of sulfur vacancies-enriched heterogeneous catalysts for efficiently activating PMS for refractory organic pollutants elimination.
Published Version
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