标题：Theoretical investigation on the contribution of HO[rad], SO4[rad]- and CO3[rad]- radicals to the degradation of phenacetin in water: Mechanisms, kinetics, and toxicity evaluation
作者：Li M.; Sun J.; Han D.; Wei B.; Mei Q.; An Z.; Wang X.; Cao H.;等 更多 作者机构：[Li, M] Environment Research Institute, Shandong University, Qingdao, 266237, China;[ Sun, J] Environment Research Institute, Shandong University, Qin 更多
通讯作者地址：[He, M] Environment Research Institute, Shandong UniversityChina;
来源：Ecotoxicology and Environmental Safety
关键词：Aquatic toxicity; Degradation mechanism; Density functional theory; Rate constants; Simulated water treatment
摘要：Indirect oxidation induced by reactive free radicals, such as hydroxyl radical (HO[rad]), sulfate radical (SO4[rad]-) and carbonate radical (CO3[rad]-), plays an important or even crucial role in the degradation of micropollutants. Thus, the coadjutant degradation of phenacetin (PNT) by HO[rad], SO4[rad]- and CO3[rad]-, as well as the synergistic effect of O2 on HO[rad] and HO2 were studied through mechanism, kinetics and toxicity evaluation. The results showed that the degradation of PNT was mainly caused by radical adduct formation (RAF) reaction (69% for Г, the same as below) and H atom transfer (HAT) reaction (31%) of HO[rad]. For the two inorganic anionic radicals, SO4[rad]- initiated PNT degradation by sequential radical addition-elimination (SRAE; 55%), HAT (28%) and single electron transfer (SET; 17%) reactions, while only by HAT reaction for CO3[rad]-. The total initial reaction rate constants of PNT by three radicals were in the order: SO4[rad]- > HO[rad] > CO3[rad]-. The kinetics of PNT degradation simulated by Kintecus program showed that UV/persulfate could degrade target compound more effectively than UV/H2O2 in ultrapure water. In the subsequent reaction of PNT with O2, HO[rad] and HO2, the formation of mono/di/tri-hydroxyl substitutions and unsaturated aldehydes/ketones/alcohols were confirmed. The results of toxicity assessment showed that the acute and chronic toxicity of most products to fish increased and to daphnia decreased, and acute toxicity to green algae decreased while chronic toxicity increased. © 2020 Elsevier Inc.