Jans Urs, Prasse Carsten, von Gunten Urs
Department of Chemistry and Biochemistry, The City College of New York, New York, New York 10031, United States.
Chemistry Program, Graduate School and University Center of the City University of New York, New York, New York 10016, United States.
Environ Sci Technol. 2021 Mar 2;55(5):3313-3321. doi: 10.1021/acs.est.0c07662. Epub 2021 Feb 15.
Combining iron with a tetraamido-macrocyclic ligand (Fe-TAML) as a catalyst and with hydrogen peroxide (HO) as the bulk oxidant is a process that has been suggested for the oxidative abatement of micropollutants during water treatment. In this study, the reactivity of the Fe-TAML/HO system was evaluated by investigating the degradation of a group of electron-rich organic model compounds with different functional groups in a secondary wastewater effluent. Phenolic compounds and a polyaromatic ether are quickly and substantially abated by Fe-TAML/HO in a wastewater effluent. For tertiary amines, a moderate rate of abatement was observed. Primary and secondary amines, aromatic ethers, aromatic aldehydes, and olefins are oxidized too slowly in the investigated Fe-TAML/HO systems to be significantly abated in a secondary wastewater effluent. Trichlorophenol is readily oxidized to chloromaleic acid and chlorofumaric acid, which support a one-electron transfer reaction as the initial step of the reaction between Fe-TAML/HO and the target compound. Fe-TAML/HO does not oxidize bromide to hypobromous acid; however, iodide is oxidized to hypoiodous acid, and as a consequence, the HO consumption is accelerated by a catalytic reaction in iodide-containing water. Overall, Fe-TAML/HO is a rather selective oxidant, which makes it an interesting system for the abatement of electron-rich phenolic-type pollutants.
将铁与四酰胺大环配体(Fe-TAML)作为催化剂,并与过氧化氢(H₂O₂)作为大量氧化剂相结合,是一种在水处理过程中用于氧化去除微污染物的方法。在本研究中,通过研究二级废水流出物中一组具有不同官能团的富电子有机模型化合物的降解情况,评估了Fe-TAML/H₂O₂体系的反应活性。酚类化合物和一种多芳醚在废水流出物中能被Fe-TAML/H₂O₂快速且大量地去除。对于叔胺,观察到了适度的去除速率。伯胺和仲胺、芳醚、芳醛以及烯烃在研究的Fe-TAML/H₂O₂体系中氧化速度过慢,在二级废水流出物中无法被显著去除。三氯苯酚很容易被氧化为氯马来酸和氯富马酸,这支持了单电子转移反应作为Fe-TAML/H₂O₂与目标化合物反应的初始步骤。Fe-TAML/H₂O₂不会将溴化物氧化为次溴酸;然而,碘化物会被氧化为次碘酸,因此,在含碘水中,通过催化反应加速了H₂O₂的消耗。总体而言,Fe-TAML/H₂O₂是一种相当有选择性的氧化剂,这使其成为去除富电子酚类污染物的一个有趣体系。