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Communication

Evoked Methane Photocatalytic Conversion to C2 Oxygenates over Ceria with Oxygen Vacancy

1
College of Sciences, Shanghai University, Shanghai 200444, China
2
CAS Key Laboratory of Low-carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China
3
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
*
Authors to whom correspondence should be addressed.
Catalysts 2020, 10(2), 196; https://doi.org/10.3390/catal10020196
Submission received: 27 December 2019 / Revised: 17 January 2020 / Accepted: 31 January 2020 / Published: 6 February 2020

Abstract

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.
Keywords: ceria; oxygen vacancy; photocatalysis; methane conversion ceria; oxygen vacancy; photocatalysis; methane conversion

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MDPI and ACS Style

Du, J.; Chen, W.; Wu, G.; Song, Y.; Dong, X.; Li, G.; Fang, J.; Wei, W.; Sun, Y. Evoked Methane Photocatalytic Conversion to C2 Oxygenates over Ceria with Oxygen Vacancy. Catalysts 2020, 10, 196. https://doi.org/10.3390/catal10020196

AMA Style

Du J, Chen W, Wu G, Song Y, Dong X, Li G, Fang J, Wei W, Sun Y. Evoked Methane Photocatalytic Conversion to C2 Oxygenates over Ceria with Oxygen Vacancy. Catalysts. 2020; 10(2):196. https://doi.org/10.3390/catal10020196

Chicago/Turabian Style

Du, Jin, Wei Chen, Gangfeng Wu, Yanfang Song, Xiao Dong, Guihua Li, Jianhui Fang, Wei Wei, and Yuhan Sun. 2020. "Evoked Methane Photocatalytic Conversion to C2 Oxygenates over Ceria with Oxygen Vacancy" Catalysts 10, no. 2: 196. https://doi.org/10.3390/catal10020196

APA Style

Du, J., Chen, W., Wu, G., Song, Y., Dong, X., Li, G., Fang, J., Wei, W., & Sun, Y. (2020). Evoked Methane Photocatalytic Conversion to C2 Oxygenates over Ceria with Oxygen Vacancy. Catalysts, 10(2), 196. https://doi.org/10.3390/catal10020196

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