Partial oxidation of methane to methyl oxygenates with enhanced selectivity using a single-atom copper catalyst on amorphous carbon support

In this study, we report a single-atom Cu catalyst on the amorphous carbon support for direct methane partial oxidation. The catalyst was prepared by the carbonization of Cu-doped ZIF-8 to implant single-atom Cu active centers that coordinate with four nitrogen (CuN4) on the amorphous N-doped carbon. Carbonization enhanced the oxidation resistance of the catalyst by preventing the oxidation of Cu-coordinating ligands, leading to a 40% reduction in CO2 production. Our prepared catalyst showed higher methanol selectivity than other single-atom copper catalysts. Mechanistic studies revealed that Cu and the surface carbon atom facilitated the dissociation of H2O2 into OOH and H, which further transformed into Cu-O and led to proton abstraction from methane. We highlight a simple approach to prepare a single-atom catalyst that is supported on amorphous N-doped carbon, derived from a metal-doped ZIF. This catalyst exhibits enhanced selectivity and stability for the partial oxidation of methane.

Automated summary

In this study, a single-atom Cu catalyst supported on amorphous carbon was prepared for direct methane partial oxidation. Carbonization of Cu-doped ZIF-8 resulted in the implantation of single-atom Cu active centers on the amorphous N-doped carbon. The prepared catalyst exhibited high selectivity and stability for methane oxidation.