Université Paris-Est, Laboratoire Géomatériaux et Environnement (LGE), EA 4508, Marne-la-Vallée, France.
Environ Sci Technol. 2012 Apr 3;46(7):4074-82. doi: 10.1021/es204621q. Epub 2012 Mar 12.
The electro-Fenton treatment of sulfachloropyridazine (SCP), a model for sulfonamide antibiotics that are widespread in waters, was performed using cells with a carbon-felt cathode and Pt or boron-doped diamond (BDD) anode, aiming to present an integral assessment of the kinetics, electrodegradation byproducts, and toxicity evolution. H(2)O(2) electrogeneration in the presence of Fe(2+) yielded (•)OH in the solution bulk, which acted concomitantly with (•)OH adsorbed at the anode (BDD((•)OH)) to promote the oxidative degradation of SCP (k(abs,SCP) = (1.58 ± 0.02) × 10(9) M(-1) s(-1)) and its byproducts. A detailed scheme for the complete mineralization was elucidated. On the basis of the action of (•)OH onto four different SCP sites, the pathways leading to total decontamination includes fifteen cyclic byproducts identified by HPLC and GC-MS, five aliphatic carboxylic acids, and a mixture of Cl(-), SO(4)(2-), NH(4)(+), and NO(3)(-) that accounted for 90-100% of initial Cl, S, and N. The time course of byproducts was satisfactorily correlated with the toxicity profiles determined from inhibition of Vibrio fischeri luminescence. 3-Amino-6-chloropyridazine and p-benzoquinone were responsible for the increased toxicity during the first stages. Independent electrolyses revealed that their toxicity trends were close to those of SCP. The formation of the carboxylic acids involved a sharp toxicity decrease, thus ensuring overall detoxification.
用电芬顿法处理磺胺氯哒嗪(SCP),这是一种广泛存在于水中的磺胺类抗生素的模型化合物,使用带有碳纤维毡阴极和 Pt 或掺硼金刚石(BDD)阳极的细胞进行处理,旨在对动力学、电极降解副产物和毒性演变进行综合评估。在 Fe(2+)存在下产生 H(2)O(2)会在溶液主体中生成 (•)OH,它与吸附在阳极上的 (•)OH (BDD((•)OH))共同作用,促进 SCP 的氧化降解(k(abs,SCP) = (1.58 ± 0.02) × 10(9) M(-1) s(-1))及其副产物。阐明了完全矿化的详细方案。基于 (•)OH 对 SCP 的四个不同位点的作用,导致完全净化的途径包括通过 HPLC 和 GC-MS 鉴定的十五个环状副产物,五个脂肪族羧酸,以及 Cl(-)、SO(4)(2-)、NH(4)(+)和 NO(3)(-)的混合物,它们占初始 Cl、S 和 N 的 90-100%。副产物的时间过程与通过抑制发光菌发光测定的毒性谱非常相关。3-氨基-6-氯哒嗪和对苯醌在最初阶段导致毒性增加。独立电解表明它们的毒性趋势与 SCP 相似。羧酸的形成涉及毒性急剧下降,从而确保整体解毒。