Selective Oxidation of Methane to Methanol over Au/H-MOR

Wangyang Wang; Wei Zhou; Yuchen Tang; Weicheng Cao; Scott R Docherty; Fangwei Wu; Kang Cheng; Qinghong Zhang; Christophe Copéret; Ye Wang

doi:10.1021/jacs.3c04260

Selective Oxidation of Methane to Methanol over Au/H-MOR

J Am Chem Soc. 2023 Jun 14;145(23):12928-12934. doi: 10.1021/jacs.3c04260. Epub 2023 Jun 2.

Authors

Wangyang Wang¹, Wei Zhou^{1

2}, Yuchen Tang¹, Weicheng Cao^{2

3}, Scott R Docherty², Fangwei Wu¹, Kang Cheng¹, Qinghong Zhang¹, Christophe Copéret², Ye Wang¹

Affiliations

¹ 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.
² Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 2, CH-8093 Zürich, Switzerland.
³ Department of Chemistry, Zhejiang University, Hangzhou 310027, China.

PMID: 37267262
DOI: 10.1021/jacs.3c04260

Abstract

Selective oxidation of methane to methanol by dioxygen (O₂) 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.