文献类型：期刊文献

英文题名：Semiconducting mineral induced photochemical conversion of PAHs in aquatic environment: Mechanism study and fate prediction

作者：Cai, Zhengqing[1,2];Yang, Fuquan[1];Song, Yanyu[1];Liu, Yongdi[1];Liu, Wen[3];Wang, Qilin[4];Sun, Xianbo[1]

机构：[1]East China Univ Sci & Technol, Natl Engn Res Ctr Ind Wastewater Detoxicat & Resou, Shanghai 200237, Peoples R China;[2]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200237, Peoples R China;[3]Peking Univ, Minist Educ Coll Environm Sci & Engn, Key Lab Water & Sediment Sci, Beijing 100871, Peoples R China;[4]Univ Technol Sydney, Ctr Technol Water & Wastewater, Sch Civil & Environm Engn, Ultimo, NSW 2007, Australia

年份：2023

卷号：860

外文期刊名：SCIENCE OF THE TOTAL ENVIRONMENT

收录：;EI(收录号：20224913215661);WOS:【SCI-EXPANDED(收录号:WOS:000919595400001)】；

基金：Acknowledgments This work was supported by the Natural Science Foundation of Shang-hai [21ZR1415600] , the National Natural Science Foundation of China [41807340] .

语种：英文

外文关键词：Natural weathering; Natural semiconductors; Photocatalytic; Fenton; PAHs

摘要：Semiconducting minerals (such as iron sulfides) are highly abundant in surface water, but their influences on the natural photochemical process of contaminants are still unknown. By simulating the natural water environment under solar irra-diation, this work comprehensively investigated the photochemical processes of anthracene (a typical Polycyclic Aromatic Hydrocarbons) in both freshwater and seawater. The results show that the natural pyrite (NP) significantly promotes the degradation of anthracene under solar illumination via 1) NP induced photocatalytic degradation of anthracene, and 2) Fenton reaction due to the NP induced photocatalytic generation of H2O2. The material characterization and theoretical calculation reveal that the natural impurity in NP enlarges its band gap, which limits the utilization of solar spectra to shorter wavelength. The contribution of generated reactive intermediates on anthracene degradation follows the order of 1O2 > center dot OH > O2 center dot- in freshwater and O2 center dot- > 1O2 > center dot OH in seawater. The photochemically generated H2O2 is a vital source for center dot OH generation (from Fenton reaction). The steady-state concentration of center dot OH, 1O2 and O2 center dot- in freshwater were mon-itored as 3.0 x 10-15M, 1.1 x 10-13 M, and 4.5 x 10-14M, respectively. However, the center dot OH concentration in seawater can be negligible due to the quenching effects by halides, and the 1O2 and O2 center dot- concentrations are higher than that in fresh-water. An anthracene degradation kinetic model was built based on the experimentally determined reactive intermediates concentration and its second order rate constant with anthracene. Moreover, the anthracene degradation pathway was proposed based on intermediates analysis and DFT calculation, and its toxicity evolution during the photochemical pro-cess was assessed by quantitative structure-activity relationship (QSAR) based prediction. This finding suggests that the natural semiconducting minerals can affect the fate and environmental risks of contaminants in natural water.