2D Spatial Structure Favored Tandem Catalysis Boosted Methane Direct Transformation to Methanol over Cu-FER

Abstract

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