The University of Queensland, Brisbane, QLD Advanced Water Management Centre, 4072, Australia.
Water Res. 2011 May;45(10):3205-14. doi: 10.1016/j.watres.2011.03.040. Epub 2011 Mar 29.
Electrochemical oxidation has been proposed for the elimination of pesticides, pharmaceuticals and other organic micropollutants from complex waste streams. However, the detrimental effect of halide ion mediators and the generation of halogenated by-products in this process have largely been neglected thus far. In this study, we investigated the electrochemical oxidation pathways of the β-blocker metoprolol in reverse osmosis concentrate (ROC) from a water reclamation plant using titanium anodes coated with Ru(0.7)Ir(0.3)O(2) or SnO(2)-Sb metal oxide layers. The results of liquid chromatography-mass spectrometry analysis indicated that irrespective of the electrode coating the same oxidant species participated in electrochemical transformation of metoprolol in ROC. Although Ti/SnO(2)-Sb exhibited higher oxidizing power for the same applied specific electrical charge, the generation of large fractions of chloro-, chloro-bromo- and bromo derivatives was observed for both electrode coatings. However, degradation rates of metoprolol and its degradation products were generally higher for the Ti/SnO(2)-Sb anode. Chemical analyses of metoprolol and its by-products were complemented with bioanalytical tools in order to investigate their toxicity relative to the parent compound. Results of the bioluminescence inhibition test with Vibrio fischeri and the combined algae test with Pseudokirchneriella subcapitata indicated a substantial increase in non-specific toxicity of the reaction mixture due to the formed halogenated by-products, while the specific toxicity (inhibition of photosynthesis) remained unchanged.
电化学氧化已被提议用于消除复杂废水中的农药、药物和其他有机微量污染物。然而,迄今为止,卤化物离子介质的有害影响以及该过程中卤代副产物的产生在很大程度上被忽视了。在这项研究中,我们使用涂有 Ru(0.7)Ir(0.3)O(2)或 SnO(2)-Sb 金属氧化物层的钛阳极研究了来自水回收厂的反渗透浓缩物(ROC)中β受体阻滞剂美托洛尔的电化学氧化途径。液相色谱-质谱分析的结果表明,无论电极涂层如何,相同的氧化剂物种都参与了 ROC 中美托洛尔的电化学转化。尽管 Ti/SnO(2)-Sb 对相同的施加比电荷表现出更高的氧化能力,但两种电极涂层都观察到氯、氯溴和溴代衍生物的大分数生成。然而,美托洛尔及其降解产物的降解速率通常对于 Ti/SnO(2)-Sb 阳极更高。美托洛尔及其副产物的化学分析辅以生物分析工具,以研究它们相对于母体化合物的毒性。发光细菌抑制试验和 Pseudokirchneriella subcapitata 藻类联合试验的结果表明,由于形成的卤代副产物,反应混合物的非特异性毒性显著增加,而特异性毒性(光合作用抑制)保持不变。