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

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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 g_catalyst⁻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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