Switchable single-atom catalysts for highly selective C–C coupling in direct methane oxidation

Authors:
Publisher website
Google Scholar
Abstract
Direct selective conversion of methane into high value-added chemical products has long attracted attention in both industry and academia. The production of C2 oxygenates is especially challenging owing to the requirement for both C–H activation and C–C coupling. Here we report a boron nanosheet-supported Cu single atom with Cu–B4 sites (Cu-SAs/B), which can effectively catalyse the conversion of methane to acetic acid with 97% selectivity and a high activity of 221.3 mmol gCu−1 h−1 without the addition of CO. In situ X-ray absorption fine structure analysis reveals that Cu single atoms undergo reversible ‘switching’ to Cu4 clusters under CH4 oxidation conditions, enabling efficient C–H activation and C–C coupling. The switching behaviour is triggered by the presence of H2O2, and the coupling occurs between CH3* and CHO* intermediates formed on Cu single atoms and Cu clusters, respectively, as confirmed by in situ spectroscopic techniques. These findings provide a proof of concept for designing highly effective methane oxidation catalysts based on switchable nanocatalysts.

This publication has 52 references indexed in Scilit: