Stoichiometric methane conversion to ethane using photochemical looping at ambient temperature

Xiang Yu, Vladimir L. Zholobenko, Simona Moldovan, Di Hu, Dan Wu, Vitaly V. Ordomsky () and Andrei Y. Khodakov ()
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Xiang Yu: UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide
Vladimir L. Zholobenko: Keele University
Simona Moldovan: CNRS, Université Normandie and INSA Rouen Avenue de l’Université-BP12
Di Hu: UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide
Dan Wu: UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide
Vitaly V. Ordomsky: UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide
Andrei Y. Khodakov: UMR 8181 – UCCS – Unité de Catalyse et Chimie du Solide

Nature Energy, 2020, vol. 5, issue 7, 511-519

Abstract: Abstract Methane activation and utilization are among the major challenges of modern science. Methane is potentially an important feedstock for manufacturing value-added fuels and chemicals. However, most known processes require excessive operating temperatures and exhibit insufficient selectivity. Here, we demonstrate a photochemical looping strategy for highly selective stoichiometric conversion of methane to ethane at ambient temperature over silver–heteropolyacid–titania nanocomposites. The process involves a stoichiometric reaction of methane with highly dispersed cationic silver under illumination, which results in the formation of methyl radicals. Recombination of the generated methyl radicals leads to the selective, and almost quantitative, formation of ethane. Cationic silver species are simultaneously reduced to metallic silver. The silver–heteropolyacid–titania nanocomposites can be reversibly regenerated in air under illumination at ambient temperature. The photochemical looping process achieves a methane coupling selectivity of over 90%, a quantitative yield of ethane of over 9%, high quantum efficiency (3.5% at 362 nm) and excellent stability.

Date: 2020
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DOI: 10.1038/s41560-020-0616-7

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