Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane

Yihong Chen; Yuan Zhao; Dong Liu; Gang Wang; Wenbin Jiang; Shengkun Liu; Wenqing Zhang; Yaping Li; Zili Ma; Tianyi Shao; Hengjie Liu; Xiyu Li; Zhiyong Tang; Chao Gao; Yujie Xiong

doi:10.1021/jacs.3c10069

Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane

J Am Chem Soc. 2024 Jan 31;146(4):2465-2473. doi: 10.1021/jacs.3c10069. Epub 2024 Jan 17.

Authors

Yihong Chen^{1

2}, Yuan Zhao^{1

3}, Dong Liu^{1

2}, Gang Wang⁴, Wenbin Jiang⁵, Shengkun Liu¹, Wenqing Zhang¹, Yaping Li¹, Zili Ma¹, Tianyi Shao¹, Hengjie Liu¹, Xiyu Li^{1

3}, Zhiyong Tang^{4

6}, Chao Gao¹, Yujie Xiong^{1

2

6}

Affiliations

¹ Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovative Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, School of Nuclear Science and Technology, and Center for Micro- and Nanoscale Research and Fabrication, University of Science and Technology of China, Hefei 230026, China.
² Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu 215123, China.
³ Songshan Lake Materials Laboratory, Dongguan, Guangdong 523808, China.
⁴ CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, China.
⁵ Institute of Materials Research and Engineering, A*STAR, Singapore 138634, Singapore.
⁶ Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Engineering Research Center of Carbon Neutrality, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241000, China.

PMID: 38232304
DOI: 10.1021/jacs.3c10069

Abstract

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.