Highly efficient light-driven methane coupling under ambient conditions based on an integrated design of a photocatalytic system

Direct non-oxidative coupling of methane (NOCM) is an effective way to produce hydrocarbons. However, this process usually requires a high temperature (≥1100 °C) to break the C-H bond of CH 4 and suffers catalyst deactivation due to coke formation. Photocatalytic NOCM is an ideal strategy to solve t...

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Published inGreen chemistry : an international journal and green chemistry resource : GC Vol. 22; no. 14; pp. 4669 - 4675
Main Authors Lang, Junyu, Ma, Yuli, Wu, Xuechen, Jiang, Yueyue, Hu, Yun Hang
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 01.01.2020
Subjects
Catalysts
Continuous flow
Coupling
Deactivation
Ethane
Gold
Green chemistry
High temperature
Hydrogen bonds
Irradiation
Light reflection
Methane
Photocatalysis
Photoelectrons
Radiation
Recombination
Room temperature
Selectivity
Temperature requirements
Titanium dioxide
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Summary:Direct non-oxidative coupling of methane (NOCM) is an effective way to produce hydrocarbons. However, this process usually requires a high temperature (≥1100 °C) to break the C-H bond of CH 4 and suffers catalyst deactivation due to coke formation. Photocatalytic NOCM is an ideal strategy to solve these issues. Herein, we designed a novel photocatalytic methane coupling system consisting of a continuous flow reactor and metal-loaded TiO 2 photocatalysts with light-diffuse-reflection-surfaces. It was found that Au/TiO 2 was the best catalyst for the system due to the easy transport of photoelectrons from TiO 2 to Au particles to inhibit the photoelectron-hole recombination. The yield of C 2 H 6 reached 81.7 μmol g catalyst −1 h −1 with higher than 95% selectivity over Au/TiO 2 under simulated 1.5G sunlight irradiation and ambient conditions (room temperature and 1 atm), which is 174% larger than the highest reported value. Furthermore, DFT calculation results revealed that the methyl anion is a possible intermediate species for the formation of ethane. A novel photocatalytic system for highly efficient non-oxidative coupling of methane was demonstrated by dispersing a metal loaded TiO 2 catalyst on the light-diffuse-reflection surface with a continuous flow reactor.
Bibliography:10.1039/d0gc01608j
Electronic supplementary information (ESI) available: Detailed description of the experimental methods and additional data and figures. See DOI
ISSN:1463-9262
1463-9270
DOI:10.1039/d0gc01608j