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J Hazard Mater


Title:Tuning the olefin-VOCs epoxidation performance of ceria by mechanochemical loading of coinage metal
Author(s):Xiong C; Xue C; Yu X; He Y; Liang Y; Zhou X; Ji H;
Address:"Fine Chemical Industry Research Institute, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, PR China. School of Chemical Engineering and Technology, Sun Yat-Sen University, Zhuhai 519082, PR China; Guangdong Provincial Key Laboratory of Optical Chemicals, XinHuaYue Group, Maoming 525000, PR China. Electronic address: xuecan@mail.sysu.edu.cn. School of Chemical Engineering and Technology, Sun Yat-Sen University, Zhuhai 519082, PR China. Fine Chemical Industry Research Institute, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, PR China; Advanced Energy Science and Technology Guangdong Laboratory, Huizhou 516000, PR China. Electronic address: jihb@mail.sysu.edu.cn"
Journal Title:J Hazard Mater
Year:2023
Volume:20220903
Issue:
Page Number:129888 -
DOI: 10.1016/j.jhazmat.2022.129888
ISSN/ISBN:1873-3336 (Electronic) 0304-3894 (Linking)
Abstract:"Under the background of carbon dioxide emission reduction, how to realize the treatment and the high value-added conversion of typical olefin volatile organic compounds (olefin-VOCs), such as styrene, is a big challenge. In this contribution, the ceria-supported coinage metal catalysts (M/CeO(2), M = Au, Ag, and Cu) are successfully synthesized by a dry mechanochemical method, and their catalytic performance for styrene-VOC epoxidation with tert-butyl hydrogen peroxide (TBHP) as an oxidant to prepare high-value styrene oxide (SO) is investigated. The oxygen vacancies of ceria play a key role in the anchoring of metal nanoparticles. After ball milling, Au(III) is partially reduced and coexists on ceria in two valence states (Au(3+) and Au(0)), and the reactive oxygen species of the as-prepared catalyst are enhanced. The catalytic behaviors, including solvents effect, substrate concentration, oxidant ratio, catalyst dosage, reaction time, and temperature, are systematically investigated. Au/CeO(2) exhibits good styrene epoxidation performance with a total styrene conversion of 94% and a SO yield of 63%, along with good reusability and substrate scalability. Thermodynamics and kinetics show that Au/CeO(2) was more favorable for styrene epoxidation and this reaction is dominated by the rate of intrinsic chemical reactions on the surface of the catalyst. Based on experimental discussions and a set of characterizations (XPS, XRD, in-situ FT-IR, ESR, ESI-HSMS, etc.), the mechanism is revealed as the synergistic catalysis between the reactive oxygen species of Au/CeO(2) and the peroxide radicals generated by the homolysis of TBHP"
Keywords:Ceria Coinage metals Mechanochemical Olefin-VOCs epoxidation Synergistic catalysis;
Notes:"PubMed-not-MEDLINEXiong, Chao Xue, Can Yu, Xingrui He, Yaorong Liang, Yichao Zhou, Xiantai Ji, Hongbing eng Netherlands 2022/09/10 J Hazard Mater. 2023 Jan 5; 441:129888. doi: 10.1016/j.jhazmat.2022.129888. Epub 2022 Sep 3"

 
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