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

被引:77
作者
Lang, Junyu [1 ]
Ma, Yuli [1 ]
Wu, Xuechen [1 ]
Jiang, Yueyue [1 ]
Hu, Yun Hang [1 ,2 ]
机构
[1] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China
[2] Michigan Technol Univ, Dept Mat Sci & Engn, Houghton, MI 49931 USA
基金
中国博士后科学基金;
关键词
SILICA; AU; AG; CATALYSTS; ETHYLENE; CLUSTERS; SURFACE; ETHANE; OXIDE; CU;
D O I
10.1039/d0gc01608j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:4669 / 4675
页数:7
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