Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane,Journal of the American Chemical Society

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Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-01-17 , DOI: 10.1021/jacs.3c10069
Yihong Chen _{1,

2} , Yuan Zhao _{1,

3} , Dong Liu _{1,

2} , Gang Wang ₄ , Wenbin Jiang ₅ , Shengkun Liu ₁ , Wenqing Zhang ₁ , Yaping Li ₁ , Zili Ma ₁ , Tianyi Shao ₁ , Hengjie Liu ₁ , Xiyu Li _{1,

3} , Zhiyong Tang _{4,

6} , Chao Gao ₁ , Yujie Xiong _{1,

2,

6}

Affiliation

Photocatalytic oxidative coupling of methane (OCM) into value-added industrial chemicals offers an appealing green technique for achieving sustainable development, whereas it encounters double bottlenecks in relatively low methane conversion rate and severe overoxidation. Herein, we engineer a continuous gas flow system to achieve efficient photocatalytic OCM while suppressing overoxidation by synergizing the moderate active oxygen species, surface plasmon-mediated polarization, and multipoint gas intake flow reactor. Particularly, a remarkable CH₄ conversion rate of 218.2 μmol h^–1 with an excellent selectivity of ∼90% toward C₂₊ hydrocarbons and a remarkable stability over 240 h is achieved over a designed Au/TiO₂ photocatalyst in our continuous gas flow system with a homemade three-dimensional (3D) printed flow reactor. This work provides an informative concept to engineer a high-performance flow system for photocatalytic OCM by synergizing the design of the reactor and photocatalyst to synchronously regulate the mass transfer, activation of reactants, and inhibition of overoxidation.

中文翻译：

用于甲烷高效、耐用光催化氧化偶联的连续流系统

甲烷光催化氧化偶联（OCM）转化为增值工业化学品为实现可持续发展提供了一种极具吸引力的绿色技术，但它遇到了甲烷转化率相对较低和严重过度氧化的双重瓶颈。在这里，我们设计了一个连续气流系统，以实现高效的光催化OCM，同时通过协同适度的活性氧、表面等离子体介导的极化和多点进气流反应器来抑制过度氧化。特别是，在我们的连续气流系统中，设计的 Au/TiO ₂光催化剂实现了 218.2 μmol h ^–1的显着 CH ₄转化率，对 C ₂₊碳氢化合物的选择性约为 90%，并且在 240 小时内具有显着的稳定性。带有自制的三维（3D）打印流动反应器。这项工作提供了一个信息丰富的概念，通过协同反应器和光催化剂的设计来设计光催化OCM的高性能流动系统，以同步调节传质、反应物的活化和过氧化的抑制。

更新日期：2024-01-17

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