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Author:

Wang, Jia (Wang, Jia.) | Dai, Lingyun (Dai, Lingyun.) | Deng, Jiguang (Deng, Jiguang.) | Liu, Yuxi (Liu, Yuxi.) | Jing, Lin (Jing, Lin.) | Pei, Wenbo (Pei, Wenbo.) | Hou, Zhiquan (Hou, Zhiquan.) | Zhang, Xing (Zhang, Xing.) | Yu, Xiaohui (Yu, Xiaohui.) | Dai, Hongxing (Dai, Hongxing.) (Scholars:戴洪兴)

Indexed by:

EI Scopus SCIE

Abstract:

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.

Keyword:

Mesoporous iron oxide-supported catalyst Density function theory Typical aromatics oxidation AuMn intermetallic compound Volatile organic compound

Author Community:

  • [ 1 ] [Wang, Jia]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 2 ] [Deng, Jiguang]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 3 ] [Liu, Yuxi]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 4 ] [Jing, Lin]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 5 ] [Pei, Wenbo]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 6 ] [Hou, Zhiquan]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 7 ] [Zhang, Xing]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 8 ] [Yu, Xiaohui]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 9 ] [Dai, Hongxing]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat,Sch Env, Key Lab Beijing Reg Air Pollut Control,Dept Envir, Minist China,Fac Environm & Life,Lab Catalysis Ch, Beijing 100124, Peoples R China
  • [ 10 ] [Dai, Lingyun]Harvard Univ, John A Paulson Sch Engn & Appl Sci, Cambridge, MA 02138 USA

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Source :

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

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