North China University of Science and Technology, Tangshan 063210, Hebei, China.
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
J Hazard Mater. 2019 Jul 5;373:85-96. doi: 10.1016/j.jhazmat.2019.03.075. Epub 2019 Mar 19.
Magnetically separable Cu/CuFeO composite obtained by a solvothermal method was used to active persulfate (PS) for the removal of tetracycline (TC). Under different pH conditions, Cu/CuFeO catalyst exhibited a higher catalytic activity for PS activation to degrade TC than that of CuFeO. The effects of some key parameters including initial pH value, PS concentration, catalyst dosage, reaction temperature and coexisting ions on TC degradation were investigated in Cu/CuFeO/PS system. The reuse of Cu/CuFeO catalyst at pH 3.50, 7.00 and 11.00 indicated that the catalyst showed a low stability due to the corrosion of metallic copper (Cu°), but bicarbonate ions could enhance the stability and recyclability of this catalyst through the suppression of copper leaching. Both sulfate and hydroxyl radicals were the main reactive species in Cu/CuFeO/PS system. Cu° can not only work as electron donor to active PS to produce the reactive radicals but also act as an electron bridge to facilitate the fast electron transfer between PS and catalyst. The structural cuprous and ferrous ions on the surface of CuFeO participated in the PS activation process through the redox reactions, as confirmed by XPS analysis. The possible degradation pathways of TC were proposed based on the identified intermediates.
采用溶剂热法制备了可分离的磁性 Cu/CuFeO 复合材料,用于激活过硫酸盐 (PS) 去除四环素 (TC)。在不同的 pH 值条件下,Cu/CuFeO 催化剂对 PS 活化降解 TC 的催化活性高于 CuFeO。在 Cu/CuFeO/PS 体系中,研究了初始 pH 值、PS 浓度、催化剂用量、反应温度和共存离子等一些关键参数对 TC 降解的影响。在 pH 值为 3.50、7.00 和 11.00 时,Cu/CuFeO 催化剂的重复使用表明,由于金属铜 (Cu°) 的腐蚀,催化剂的稳定性较低,但碳酸氢根离子可以通过抑制铜浸出来增强催化剂的稳定性和可回收性。在 Cu/CuFeO/PS 体系中,硫酸根自由基和羟基自由基都是主要的反应性物质。Cu°不仅可以作为电子供体来激活 PS 产生反应性自由基,还可以作为电子桥,促进 PS 和催化剂之间的快速电子转移。XPS 分析证实,表面的亚铜和亚铁离子通过氧化还原反应参与 PS 活化过程。根据鉴定出的中间体,提出了 TC 的可能降解途径。