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Highly efficient light-driven methane coupling under ambient conditions based on an integrated design of a photocatalytic system
Green Chemistry ( IF 9.3 ) Pub Date : 2020-06-22 , DOI: 10.1039/d0gc01608j
Junyu Lang 1, 2, 3, 4 , Yuli Ma 1, 2, 3, 4 , Xuechen Wu 1, 2, 3, 4 , Yueyue Jiang 1, 2, 3, 4 , Yun Hang Hu 1, 2, 3, 4, 5
Affiliation  

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 CH4 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 TiO2 photocatalysts with light-diffuse-reflection-surfaces. It was found that Au/TiO2 was the best catalyst for the system due to the easy transport of photoelectrons from TiO2 to Au particles to inhibit the photoelectron–hole recombination. The yield of C2H6 reached 81.7 μmol gcatalyst−1 h−1 with higher than 95% selectivity over Au/TiO2 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.

中文翻译:

基于光催化系统的集成设计,在环境条件下高效的光驱动甲烷偶联

甲烷的直接非氧化偶联(NOCM)是生产碳氢化合物的有效方法。但是,此过程通常需要高温(≥1100°C)才能破坏CH 4的C–H键,并且由于形成焦炭而使催化剂失活。光催化NOCM是解决这些问题的理想策略。在这里,我们设计了一种新型的光催化甲烷偶联系统,该系统由连续流反应器和具有光扩散反射表面的负载金属的TiO 2光催化剂组成。人们发现,由于光电子易于从TiO 2传输到Au粒子,从而抑制了光电子与空穴的复合,因此Au / TiO 2是该体系的最佳催化剂。C 2 H 6的产率在模拟的1.5G阳光照射和环境条件(室温和1个大气压)下,催化剂的催化选择性达到81.7μmolg催化剂-1 h -1,对Au / TiO 2的选择性高于95%,比报道的最高值高174%。此外,DFT计算结果表明,甲基阴离子是可能形成乙烷的中间物种。
更新日期:2020-07-20
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