文献类型：期刊文献

英文题名：The impact of dissolved oxygen on sulfate radical-induced oxidation of organic micro-pollutants: A theoretical study

作者：Zhang, Rui[1];Wang, Xiaoxiang[2,3];Zhou, Lei[4,5];Liu, Zhu[2,6];Crump, Doug[7]

机构：[1]Univ Jinan, Sch Resources & Environm, Jinan 250022, Shandong, Peoples R China;[2]Assoc Chinese Chemists & Chem Engineer Germany, D-67117 Limburgerhof, Germany;[3]Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resources Reuse, Nanjing 210023, Jiangsu, Peoples R China;[4]East China Univ Sci & Technol, State Environm Protect Key Lab Environm Risk Asse, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China;[5]Univ Claude Bernard Lyon 1, CNRS, Univ Lyon, IRCELYON,F 69c626, 2 Ave Albert Einstein, Villeurbanne, France;[6]Tech Univ Munich, Theoret Chem & Catalysis Res Ctr, D-85747 Garching, Germany;[7]Environm & Climate Change Canada, Natl Wildlife Res Ctr, 1125 Colonel By Dr, Ottawa, ON K1A 0H3, Canada

年份：2018

卷号：135

起止页码：144

外文期刊名：WATER RESEARCH

收录：;EI(收录号：20180804824580);WOS:【SCI-EXPANDED(收录号:WOS:000429390900015)】；

基金：This research is financially supported by the Natural Science Foundation of Shandong Province (No. ZR2016BB19) and the Natural Science Foundation of Jinan University (No. XKY1628).

语种：英文

外文关键词：Sulfate radical-advanced oxidation process; Dissolved oxygen; Organic micro-pollutants; Quantum chemical calculation; Thermodynamics and kinetics

摘要：Sulfate radical (SO4(center dot-))-induced oxidation is an important technology in advanced oxidation processes (AOPs) for the removal of pollutants. To date, few studies have assessed the effects of dissolved oxygen (DO) on the SO4 center dot(-)induced oxidation of organic micro-pollutants. In the present work, a quantum chemical calculation was used to investigate the influence of the external oxygen molecule on the Gibbs free energy (G(pollutant)) and HOMO-LUMO gap (Delta E) of 15 organic micro-pollutants representing four chemical categories. Several thermodynamic and statistical models were combined with the data from the quantum chemical calculation to illustrate the impact of DO on the oxidation of organic micropollutants by SO4(center dot-). Results indicated that the external oxygen molecule increased G(pollutant) of all studied chemicals, which implies DO has the potential to decrease the energy barrier of the SO4(center dot-)-induced oxidation and shift the chemical equilibrium of the reaction towards the side of products. From the perspective of kinetics, DO can accelerate the oxidation by decreasing Delta E of organic micro-pollutants. In addition, changes of G(pollutant) and Delta E of the SO4(center dot-)-induced oxidation were both significantly different between open-chain and aromatic chemicals, and these differences were partially attributed to the difference of polarizability of these two types of chemicals. Furthermore, we revealed that all changes of G(pollutant) and Delta E induced by DO were dependent on the DO content. Our study emphasizes the significance of DO on the oxidation of organic micro-pollutants by SO4(center dot-), and also provides a theoretical method to study the effect of components in wastewater on removal of organic pollutants in AOPs. (C) 2018 Elsevier Ltd. All rights reserved.