State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 2, CH-8093 Zürich, Switzerland.
J Am Chem Soc. 2023 Jun 14;145(23):12928-12934. doi: 10.1021/jacs.3c04260. Epub 2023 Jun 2.
Selective oxidation of methane to methanol by dioxygen (O) 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 h or 280 mmol g h 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.
通过分子氧将甲烷选择性氧化为甲醇是一种有吸引力的方法，可以将丰富的甲烷资源升级，这是化学中最具挑战性的反应之一，因为产物（甲醇）的反应性远远高于反应物（甲烷）。在这里，我们报告说，在水介质中存在一氧化碳的情况下，分散在丝光沸石上的金纳米颗粒可以有效地催化甲烷通过分子氧选择性氧化为甲醇。在 150°C 下，甲醇的产率达到 1300 μmol g h 或 280 mmol g h，选择性为 75%，优于大多数在可比条件下报道的催化剂。羟基自由基和过氧物种都参与了甲烷的活化和转化，而甲醇在金上的较低亲和力主要导致了较高的甲醇选择性。
