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Author:

Xu, Ruinian (Xu, Ruinian.) | Liu, Ning (Liu, Ning.) | Dai, Chengna (Dai, Chengna.) | Li, Yan (Li, Yan.) | Zhang, Jie (Zhang, Jie.) | Wu, Bin (Wu, Bin.) | Yu, Gangqiang (Yu, Gangqiang.) | Chen, Biaohua (Chen, Biaohua.)

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EI Scopus SCIE PubMed

Abstract:

Direct oxidation of methane to methanol (DMTM) is a big challenge in C-1 chemistry. We present a continuous N2O-DMTM investigation by simultaneously introducing 10 vol % H2O into the reaction system over Cu-BEA zeolites. Combining a D2O isotopic tracer technique and ab initio molecular dynamics (AIMD) simulation, we for the first time demonstrate that the H2O molecules can participate in the reaction through a proton transfer route, wherein the H2O molecules can build a high-speed proton transfer bridge between the generated moieties of CH3- and OH- over the evolved mono(mu-oxo) dicopper ([Cu-O-Cu](2+)) active site, thereby pronouncedly boosting the CH3OH selectivity (3.1 -> 71.6 %), productivity (16.8 -> 242.9 mu mol g(cat)(-1) h(-1)) and long-term reaction stability (10 -> 70 h) relative to the scenario of absence of H2O. Unravelling the proton transfer of H2O over the dicopper [Cu-O-Cu](2+) site would substantially contribute to highly efficient catalyst designs for the continuous DMTM.

Keyword:

direct methane to methanol zeolites proton transfer N2O ab initio calculations

Author Community:

  • [ 1 ] [Xu, Ruinian]Beijing Univ Technol, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 2 ] [Liu, Ning]Beijing Univ Technol, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 3 ] [Dai, Chengna]Beijing Univ Technol, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 4 ] [Wu, Bin]Beijing Univ Technol, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 5 ] [Yu, Gangqiang]Beijing Univ Technol, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 6 ] [Chen, Biaohua]Beijing Univ Technol, Fac Environm & Life, Beijing 100124, Peoples R China
  • [ 7 ] [Chen, Biaohua]Changzhou Univ Changzhou, Sch Petrochem Engn, Jiangsu Key Lab Adv Catalyt Mat & Technol, Changzhou 213164, Jiangsu, Peoples R China
  • [ 8 ] [Li, Yan]Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
  • [ 9 ] [Zhang, Jie]Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China

Reprint Author's Address:

  • [Liu, Ning]Beijing Univ Technol, Fac Environm & Life, Beijing 100124, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

ISSN: 1433-7851

Year: 2021

Issue: 30

Volume: 60

Page: 16634-16640

1 6 . 6 0 0

JCR@2022

ESI Discipline: CHEMISTRY;

ESI HC Threshold:96

JCR Journal Grade:1

Cited Count:

WoS CC Cited Count: 0

SCOPUS Cited Count: 49

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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