Selective oxidation of methane to methanol by dioxygen (O 2 ) is an appealing route for upgrading abundant methane resource and represents one of the most challenging reactions in chemistry due to the overwhelmingly higher reactivity of the product (methanol) versus the reactant (methane). Here, we report that gold nanoparticles dispersed on mordenite efficiently catalyze the selective oxidation of methane to methanol by molecular oxygen in aqueous medium in the presence of carbon monoxide. The methanol productivity reaches 1300 μmol g cat −1 h −1 or 280 mmol g Au −1 h −1 with 75% selectivity at 150 °C, outperforming most catalysts reported under comparable conditions. Both hydroxyl radicals and hydroperoxide species participate in the activation and conversion of methane, while it is shown that the lower affinity of methanol on gold mainly accounts for higher methanol selectivity.
Selective oxidation of methane to methanol by molecular oxygen is a fascinating route for upgrading abundant methane resource and represents one of the most challenging reactions in chemistry due to the overwhelmingly higher reactivity of the product versus the reactant. Here, we report that monometallic gold nanoparticles loaded on mordenite zeolite efficiently catalyze the selective oxidation of methane to methanol by molecular oxygen in the presence of carbon monoxide in aqueous medium. The methanol productivity reaches 1300 μmol gcat−1 h−1 or 280 mmol gAu-1 h-1 with 75% selectivity at 150 °C, outperforming most of those reported under comparable conditions. Both hydroxyl radicals and hydroperoxide species participate in the activation and conversion of methane; the lower affinity of methanol on gold mainly accounts for higher methanol selectivity.
Selective oxidation of methane to methanol by molecular oxygen is a fascinating route for upgrading abundant methane resource and represents one of the most challenging reactions in chemistry due to the overwhelmingly higher reactivity of the product versus the reactant. Here, we report that monometallic gold nanoparticles loaded on mordenite zeolite efficiently catalyze the selective oxidation of methane to methanol by molecular oxygen in the presence of carbon monoxide in aqueous medium. The methanol productivity reaches 1300 μmol gcat−1 h−1 or 280 mmol gAu-1 h-1 with 75% selectivity at 150 °C, outperforming most of those reported under comparable conditions. Both hydroxyl radicals and hydroperoxide species participate in the activation and conversion of methane; the lower affinity of methanol on gold mainly accounts for higher methanol selectivity.
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