光催化
氧合物
甲烷
催化作用
氧气
甲烷氧化偶联
光化学
材料科学
部分氧化
化学
化学工程
无机化学
有机化学
工程类
作者
Jin Du,Wei Chen,Gangfeng Wu,Yuxin Song,Dong Xiao,Guihua Li,Jianhui Fang,Wei Wei,Yuhan Sun
出处
期刊:Catalysts
[MDPI AG]
日期:2020-02-06
卷期号:10 (2): 196-196
被引量:25
标识
DOI:10.3390/catal10020196
摘要
Direct conversion of methane to its oxygenate derivatives remains highly attractive while challenging owing to the intrinsic chemical inertness of CH4. Photocatalysis arises as a promising green strategy which could stimulate water splitting to produce oxidative radicals for methane C–H activation and subsequent C–C coupling. However, synthesis of a photocatalyst with an appropriate capability of methane oxidation by water remains a challenge using an effective and viable approach. Herein, ceria nanoparticles with abundant oxygen vacancies prepared by calcinating commercial CeO2 powder at high temperatures in argon are reported to capably produce ethanol and aldehyde from CH4 photocatalytic oxidation under ambient conditions. Although high-temperature calcinations lead to lower light adsorptions and increased band gaps to some extent, deficient CeO2 nanoparticles with oxygen vacancies and surface CeIII species are formed, which are crucial for methane photocatalytic conversion. The ceria catalyst as-calcinated at 1100 °C had the highest oxygen vacancy concentration and CeIII content, achieving an ethanol production rate of 11.4 µmol·gcat−1·h−1 with a selectivity of 91.5%. Additional experimental results suggested that the product aldehyde was from the oxidation of ethanol during the photocatalytic conversion of CH4.
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