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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.
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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: 1
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