2D spatial structure-favored, tandem catalysis-boosted direct transformation of methane to methanol over Cu-FER.

The direct transformation of methane into methanol (DMTM) remains a significant challenge of C1 chemistry. Herein, we investigate continuous N2O-DMTM over Cu-FER zeolite. A two-dimensional (2D) spatial structure-favored tandem catalysis is for the first time elucidated, which leads to boosted (CH3OH + DME) productivity, corresponding to 2736 μmol gcat -1 h-1 or 58 368 mmol per molCu per h of CH3OH, and improved reaction stability (passing through a 100 h long-term test). A unique dual Cu single-atom site located at the parallel 6-membered ring (MR) of the 8 MR channel could be generated, which serves as the primary CH3OH production active site exhibiting much higher activity than the traditional monomeric [Cu]+ and Cu dimer sites. The generated CH3OH can subsequently diffuse from the 8 MR channel into a 10 MR main channel and directly react with the radicals of CH3 - and OH- to produce DME not only favoring DME production but also efficiently preventing carbon deposition. The present work highlights a tandem catalysis over Cu-FER that would substantially favor the design of other efficient catalysts for N2O-DMTM.