化学
氧合物
甲烷
选择性
甲醇
光化学
光催化
催化作用
甲烷厌氧氧化
无机化学
化学工程
有机化学
工程类
作者
Lei Luo,Zhuyu Gong,Youxun Xu,Jiani Ma,Huifen Liu,Jialiang Xing,Junwang Tang
摘要
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 O2 as the oxidant operated at ambient temperature. The optimized AuCu-ZnO photocatalyst achieves up to 11225 μmol·g-1·h-1 of primary products (CH3OH and CH3OOH) 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 O2 activation to •OOH, and simultaneously that Au is an efficient hole acceptor to enhance H2O oxidation to •OH, thus synergistically promoting charge separation and methane transformation. This work highlights the significances of co-modification with suitable dual cocatalysts on simultaneous regulation of activity and selectivity.
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