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Aromatic volatile organic compounds (VOCs) are usually pollutants to the atmosphere environment and human health. In the present work, we first adopted the co-reduction and KIT-6-templating strategies to prepare the AuxMny intermetallic compounds and mesoporous iron oxide (meso-Fe2O3), respectively, and then used the impregnation method to generate the AuxMny/meso-Fe2O3 catalysts. Catalytic performance of these materials was evaluated for benzene, toluene or o-xylene (typical aromatics) oxidation. It is found that the Au5Mn2/meso-Fe2O3 catalyst exhibited the best activity: the temperatures at benzene conversions of 50 and 90 % were 237 and 254 degrees C at a space velocity of 20,000 mL/(g h), with the TOFAu values and specific reaction rates at 210 and 230 degrees C being 1.08 and 2.29 s (1), and 6.92 and 11.58 mmol/(g(Au) s), respectively. Such excellent performance of Au5Mn2/meso-Fe2O3 was related to its well dispersed Au5Mn2 nanoparticles, high adsorbed oxygen species concentration, good low-temperature reducibility, high benzene adsorption capacity, and strong benzene adsorption. The benzene chemisorption mechanism and adsorbed oxygen species could greatly influence the oxidation of benzene. According to the first-principles calculations, we find that benzene adsorption on the surface of Au in Au5Mn2/meso-Fe2O3 was in the form of a pi bond, in which the Au could obtain electrons from benzene ring in the presence of benzene adsorption, resulting in a stronger adsorption of benzene and thus increasing the catalytic activity for benzene oxidation. The mechanism of benzene oxidation might take place via the route of benzene -> phenol -> benzoquinone -> maleate (acetate) -> carbon dioxide and water. (C) 2021 Elsevier Inc. All rights reserved.
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JOURNAL OF CATALYSIS
ISSN: 0021-9517
Year: 2021
Volume: 405
Page: 273-287
7 . 3 0 0
JCR@2022
ESI Discipline: CHEMISTRY;
ESI HC Threshold:96
JCR Journal Grade:1
Cited Count:
WoS CC Cited Count: 16
SCOPUS Cited Count: 16
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 10
Affiliated Colleges: