H2O‐Built Proton Transfer Bridge Enhances Continuous Methane Oxidation to Methanol over Cu‐BEA Zeolite

Abstract 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.