Luo, Lei; Gong, Zhuyu; Xu, Youxun; Ma, Jiani; Liu, Huifen; Xing, Jialiang; Tang, Junwang; (2022) Binary Au-Cu Reaction Sites Decorated ZnO for Selective Methane Oxidation to C1 Oxygenates with Nearly 100% Selectivity at Room Temperature. Journal of the American Chemical Society , 144 (2) pp. 740-750. 10.1021/jacs.1c09141.

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Abstract

Direct and efficient oxidation of methane to methanol and the related liquid oxygenates provides a promising pathway for sustainable chemical industry, while still remaining an ongoing challenge owing to the dilemma between methane activation and overoxidation. Here, ZnO with highly dispersed dual Au and Cu species as cocatalysts enables efficient and selective photocatalytic conversion of methane to methanol and one-carbon (C1) oxygenates using O_{2} as the oxidant operated at ambient temperature. The optimized AuCu–ZnO photocatalyst achieves up to 11225 μmol·g^{–1}·h^{–1} of primary products (CH_{3}OH and CH_{3}OOH) and HCHO with a nearly 100% selectivity, resulting in a 14.1% apparent quantum yield at 365 nm, much higher than the previous best photocatalysts reported for methane conversion to oxygenates. In situ EPR and XPS disclose that Cu species serve as photoinduced electron mediators to promote O_{2} activation to •OOH, and simultaneously that Au is an efficient hole acceptor to enhance H_{2}O activation to •OOH, and simultaneously that Au is an efficient hole acceptor to enhance H2O

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