文献类型：期刊文献

英文题名：Singlet oxygen triggered by robust bimetallic MoFe/TiO2 nanospheres of highly efficacy in solar-light-driven peroxymonosulfate activation for organic pollutants removal

作者：Dong, Chencheng[1];Bao, Yan[1];Sheng, Tian[2];Yi, Qiuying[1];Zhu, Qiaohong[1];Shen, Bin[1];Xing, Mingyang[1];Lo, Irene M. C.[3];Zhang, Jinlong[1,4]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat & Joint Int Res Lab Precis Chem &, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Mat & Dynam Chem,Sch Chem & Mol, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Anhui Normal Univ, Coll Chem & Mat Sci, Wuhu 241000, Peoples R China;[3]Hong Kong Univ Sci & Technol, Dept Civil & Environm Engn, Hong Kong, Peoples R China;[4]Yancheng Inst Technol, Sch Chem & Chem Engn, Yancheng 224051, Peoples R China

年份：2021

卷号：286

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20210609878003);WOS:【SCI-EXPANDED(收录号:WOS:000621629900003)】；

基金：This work was supported by the National Natural Science Foundation of China (21972040, 21677048, 21773062, 5171101651, 21577036), the State Key Research Development Program of China (2016YFA0204200), Shanghai Municipal Science and Technology Major Project (Grant No.2018SHZDZX03) and the Programme of Introducing Talents of Discipline to Universities (B20031, B16017). The authors thank the Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

外文关键词：Bimetallic nanoparticles; MoFe/TiO2 nanospheres; PMS; Singlet oxygen

摘要：Sulfate-radical (SO4 center dot-) based Advanced Oxidation Process (SR-AOP), which is mainly generated from peroxymonosulfate (PMS) activation, is an excellent route for water treatment. Bimetallic nanoparticles have been widely applied in electronic, chemical, biological, and mechanical fields, etc.; however, few researchers have attempted to adopt bimetallic nanoparticles in environmental remediation. Further, in recent years, element molybdenum (Mo) has addressed much more environmental field attention than ever. Although singlet oxygen (O-1(2)) generated commonly in SR-AOPs, its generation mechanism remains controversial. Hence, in this work, bimetallic MoFe/TiO2 nanospheres were rationally constructed via a facile two-step methodology. Undoubtedly, it exhibited superior performance for the degradation of organic pollutants (e.g., rhodamine, phenol, 4-chlorophenol and sulfadiazine) irradiated by simulated solar light. Both photo-generated electrons and transition metallic redox couples (i.e., Mo6+/Mo4+, Fe3+/Fe2+ and Mo4+/Fe3+) play vital roles in the PMS activation. Distinct from conventional SR-AOPs, sulfate radicals (SO4 center dot-), hydroxyl radicals ((OH)-O-center dot) and peroxymonosulfate radicals (SO5 center dot-) indeed participate in the transformation and generation of singlet oxygen (O-1(2)). With the combination of DFT calculation, the Mo sites on the bimetallic MoFe (110) facet are more favorable to adsorb PMS molecules, then followed by the dissociation of PMS progressing on the Mo sites. Electrons transferring from the Mo atoms to the Fe atoms facilitated the adsorption of the negatively charged HSO5- anions, resulting in enhanced PMS activation efficiency. Considering its novelty and generation mechanism, this work highlights the mechanism of O-1(2) generation from PMS reduction and oxidation simultaneously and furnishes theoretical support for further relevant studies.