摘要
The selective conversion of peroxymonosulfate (PMS) to singlet oxygen ( 1 O 2 ) critically depends on precise electronic structure engineering of the catalysts. The PMS electron-donating pathway enables 1 O 2 generation, but the high energy barriers associated with the initial intermediate *SO 5 •− formation result in an unsatisfactory 1 O 2 yield. Herein, Co-doped ZnO was designed by calcination of zeolitic imidazolate framework. Co doping significantly improved the visible-light response, enhanced the photogenerated carrier separation and migration of ZnO, and increased the ZnO valence band potential. These effects promoted the electron-donating reaction of PMS to produce 1 O 2 . The optimized Co-ZnO-3/vis/PMS system exhibited a 27.2-fold higher methylene blue degradation rate constant (k = 0.9871 min⁻¹) with 43.7 % total organic carbon removal within 5 min. In addition, the developed 1 O 2 -dominated oxidation system removed 83.1 % of chromaticity, 59.9 % of total phenol, and 24.8 % of chemical oxidation demand from the coking wastewater tailwater. This work provides a pathway for tailoring 1 O 2 -dominated reactive species for contaminant removal, providing a theoretical guideline for the deep treatment of coking wastewater tailwater.
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