Activation of persulfate by photoexcited dye for antibiotic degradation: Radical and nonradical reactions

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2019-11, Vol.375, p.122070, Article 122070
• Main Authors: Cai, Tao, Liu, Yutang, Wang, Longlu, Dong, Wanyue, Chen, Hui, Zeng, Wengao, Xia, Xinnian, Zeng, Guangming
• Format: Article
• Language: English
• Subjects: Antibiotic; Dye; Nonradical reaction; Persulfate; Radical reaction
• ISSN: 1385-8947; 1873-3212
• DOI: 10.1016/j.cej.2019.122070

[Display omitted] •TC-H, 2,4-DNP and NOMs can be efficiently degraded by dye- activated PS.•Both radical and nonradical reactions were discovered in Dye/PS/Vis system.•LUMO levels of dyes have great influence on PS activation.•Phenolic intermediates of dye degradation play an important role in PS activation.•Effects of dye type, dye dose, DO and pH on PS activation were identified. Despite numerous studies on peroxydisulfate (PS) activation with catalysts, the PS activation by organic contaminants themselves has been rarely reported. Here, we found that PS can be activated by dyes such as rhodamine B (RhB), eosin Y (EY) and methylene blue (MB) under visible light (Vis) irradiation, achieving simultaneous degradation of dye and antibiotics (e.g., tetracycline hydrochloride) via both radical and nonradical pathways. Experimental results demonstrated that the radical reaction was the major route, which was caused by the reduction of PS by photogenerated electrons of the dye. Dye-mediated electron transfer from pollutants to the oxidized dye (dye*+) was responsible for the nonradical reaction. Compared with EY and MB, the most negative LUMO (lowest unoccupied molecular orbital) level of RhB facilitated rapid electron transfer from RhB to PS, resulting in the highest activation efficiency. Interestingly, post-processing with base can further increase the mineralization efficiency due to the PS activation by generated phenolic intermediates of RhB degradation. This work elucidated a new pathway of PS activation and provide a new “using waste to treat waste” strategy for the disposal of dye wastewater and complex wastewater containing dye.