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H 2 O‐Built Proton Transfer Bridge Enhances Continuous Methane Oxidation to Methanol over Cu‐BEA Zeolite
Author(s) -
Xu Ruinian,
Liu Ning,
Dai Chengna,
Li Yan,
Zhang Jie,
Wu Bin,
Yu Gangqiang,
Chen Biaohua
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202105167
Subject(s) - chemistry , methanol , catalysis , zeolite , proton , methane , molecule , organic chemistry , physics , quantum mechanics
Direct oxidation of methane to methanol (DMTM) is a big challenge in C 1 chemistry. We present a continuous N 2 O‐DMTM investigation by simultaneously introducing 10 vol % H 2 O into the reaction system over Cu‐BEA zeolites. Combining a D 2 O isotopic tracer technique and ab initio molecular dynamics (AIMD) simulation, we for the first time demonstrate that the H 2 O molecules can participate in the reaction through a proton transfer route, wherein the H 2 O molecules can build a high‐speed proton transfer bridge between the generated moieties of CH 3 − and OH − over the evolved mono(μ‐oxo) dicopper ([Cu‐O‐Cu] 2+ ) active site, thereby pronouncedly boosting the CH 3 OH selectivity (3.1→71.6 %), productivity (16.8→242.9 μmol g cat −1 h −1 ) and long‐term reaction stability (10→70 h) relative to the scenario of absence of H 2 O. Unravelling the proton transfer of H 2 O over the dicopper [Cu‐O‐Cu] 2+ site would substantially contribute to highly efficient catalyst designs for the continuous DMTM.