Activation of light alkanes at room temperature and ambient pressure

Abstract

Light alkane activation under mild conditions remains a substantial challenge. Here we report an aqueous reaction system capable of selectively converting light alkanes into corresponding olefins and oxygenates at room temperature and ambient pressure using Cu powder as the catalyst and O₂ as the oxidant. In ethane activation, we achieved a combined production of ethylene and acetic acid at a rate of 2.27 mmol g_(Cu)⁻¹ h⁻¹, with a combined selectivity up to 97%. Propane is converted to propylene with a selectivity up to 94% and a production rate up to 1.83 mmol g_(Cu)⁻¹ h⁻¹, while methane is converted mainly to carbon dioxide, methanol and acetic acid. On the basis of catalytic experiments, isotopic labelling experiments, spectroscopic insights and density functional theory calculations, we put forward mechanistic understandings in which the C–H bond is activated by the surface oxide species generated during the oxidation process, forming alkyl groups as key reaction intermediates.

Group Members

William A. Goddard III

Charles and Mary Ferkel Professor