Coupling conversion of methane with carbon monoxide via carbonylation over Zn/HZSM-5 catalysts

Abstract

Efficient direct transformation of methane into value-added chemicals has great significance for long-term sustainability of fuels and chemicals, but remains a major challenge due to its high inertness. Reported here is that methane can be activated effectively via carbonylation with CO over Zn/HZSM-5 catalysts under mild conditions. The selectivity to aromatics alone reaches 80% among all hydrocarbon products at 823 K, whereas as high as 92% ethane selectivity is achieved at a lower temperature of 673 K. ¹³CO isotope labelling experiments demonstrate that approximately 50% of the carbon atoms in all the products originate from carbon monoxide, whereas another half of the carbons come from methane, indicating that the precursors of hydrocarbon products are acyl compounds and/or acetic acid formed by carbonylation of methane with carbon monoxide. This provides potential for transformation of methane into value-added chemicals under mild reaction conditions.