UNESP - Univ Estadual Paulista, Instituto de Química de Araraquara, CP 355, 14801-970, Araraquara, SP, Brazil.
Water Res. 2011 Jan;45(3):1394-402. doi: 10.1016/j.watres.2010.10.029. Epub 2010 Oct 31.
The influence of iron species on amoxicillin (AMX) degradation, intermediate products generated and toxicity during the photo-Fenton process using a solar simulator were evaluated in this work. The AMX degradation was favored in the presence of the potassium ferrioxalate complex (FeOx) when compared to FeSO(4). Total oxidation of AMX in the presence of FeOx was obtained after 5 min, while 15 min were necessary using FeSO(4). The results obtained with Daphnia magna biossays showed that the toxicity decreased from 65 to 5% after 90 min of irradiation in the presence of FeSO(4). However, it increased again to a maximum of 100% after 150 min, what indicates the generation of more toxic intermediates than AMX, reaching 45% after 240 min. However, using FeOx, the inhibition of mobility varied between 100 and 70% during treatment, probably due to the presence of oxalate, which is toxic to the neonates. After 240 min, between 73 and 81% TOC removal was observed. Different pathways of AMX degradation were suggested including the opening of the four-membered β-lactamic ring and further oxidations of the methyl group to aldehyde and/or hydroxylation of the benzoic ring, generating other intermediates after bound cleavage between different atoms and further oxidation to carboxylates such acetate, oxalate and propionate, besides the generation of nitrate and ammonium.
本工作评价了铁物种在模拟太阳光照下芬顿工艺中对阿莫西林(AMX)降解、生成中间产物和毒性的影响。与 FeSO4 相比,含钾草酸盐配合物(FeOx)的存在有利于 AMX 的降解。在 FeOx 的存在下,5 分钟后即可实现 AMX 的完全氧化,而使用 FeSO4 则需要 15 分钟。用大型蚤生物测定法得到的结果表明,在 FeSO4 存在下照射 90 分钟后,毒性从 65%降至 5%。然而,在 150 分钟后,毒性又增加到 100%,这表明生成了比 AMX 更具毒性的中间产物,在 240 分钟后达到 45%。然而,使用 FeOx 时,在处理过程中,迁移率的抑制在 100%和 70%之间变化,这可能是由于草酸盐的存在,草酸盐对幼体有毒。在 240 分钟后,观察到 73%至 81%的 TOC 去除率。提出了 AMX 降解的不同途径,包括四元β-内酰胺环的打开,以及进一步对甲基进行氧化为醛和/或对苯环进行羟基化,在不同原子之间的键断裂后生成其他中间产物,并进一步氧化为羧酸根,如乙酸盐、草酸盐和丙酸盐,以及硝酸盐和铵盐的生成。