Journal
GREEN CHEMISTRY
Volume 22, Issue 14, Pages 4669-4675Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0gc01608j
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Funding
- China Postdoctoral Science Foundation [2019M651397]
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Direct non-oxidative coupling of methane (NOCM) is an effective way to produce hydrocarbons. However, this process usually requires a high temperature (>= 1100 degrees 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 mu mol 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.
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