Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis.

Abstract

Rationally constructing atom-precise active sites is highly important to promote their catalytic performance but still challenging. Herein, this work designs and constructs ZSM-5 supported Cu and Ag dual single atoms as a proof-of-concept catalyst (Ag1 -Cu1 /ZSM-5 hetero-SAC (single-atom catalyst)) to boost direct oxidation of methane (DOM) by H2 O2 . The Ag1 -Cu1 /ZSM-5 hetero-SAC synthesized via a modified co-adsorption strategy yields a methanol productivity of 20,115 µmol gcat -1 with 81% selectivity at 70°C within 30min, which surpasses most of the state-of-the-art noble metal catalysts. The characterization results prove that the synergistic interaction between silver and copper facilitates the formation of highly reactive surface hydroxyl species to activate the C-H bond as well as the activity, selectivity, and stability of DOM compared with SACs, which is the key to the enhanced catalytic performance. This work believes the atomic-level design strategy on dual-single-atom active sites should pave the way to designing advanced catalysts for methane conversion.