High-performance photocatalytic nonoxidative conversion of methane to ethane and hydrogen by heteroatoms-engineered TiO2

Wenqing Zhang, Cenfeng Fu, Jingxiang Low, Delong Duan, Jun Ma, Wenbin Jiang, Yihong Chen, Hengjie Liu, Zeming Qi, Ran Long (), Yingfang Yao (), Xiaobao Li, Hui Zhang, Zhi Liu, Jinlong Yang, Zhigang Zou and Yujie Xiong ()
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Wenqing Zhang: University of Science and Technology of China
Cenfeng Fu: University of Science and Technology of China
Jingxiang Low: University of Science and Technology of China
Delong Duan: University of Science and Technology of China
Jun Ma: University of Science and Technology of China
Wenbin Jiang: University of Science and Technology of China
Yihong Chen: University of Science and Technology of China
Hengjie Liu: University of Science and Technology of China
Zeming Qi: University of Science and Technology of China
Ran Long: University of Science and Technology of China
Yingfang Yao: Nanjing University
Xiaobao Li: ShanghaiTech University
Hui Zhang: ShanghaiTech University
Zhi Liu: ShanghaiTech University
Jinlong Yang: University of Science and Technology of China
Zhigang Zou: Nanjing University
Yujie Xiong: University of Science and Technology of China

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Nonoxidative coupling of methane (NOCM) is a highly important process to simultaneously produce multicarbons and hydrogen. Although oxide-based photocatalysis opens opportunities for NOCM at mild condition, it suffers from unsatisfying selectivity and durability, due to overoxidation of CH4 with lattice oxygen. Here, we propose a heteroatom engineering strategy for highly active, selective and durable photocatalytic NOCM. Demonstrated by commonly used TiO2 photocatalyst, construction of Pd–O4 in surface reduces contribution of O sites to valence band, overcoming the limitations. In contrast to state of the art, 94.3% selectivity is achieved for C2H6 production at 0.91 mmol g–1 h–1 along with stoichiometric H2 production, approaching the level of thermocatalysis at relatively mild condition. As a benchmark, apparent quantum efficiency reaches 3.05% at 350 nm. Further elemental doping can elevate durability over 24 h by stabilizing lattice oxygen. This work provides new insights for high-performance photocatalytic NOCM by atomic engineering.

Date: 2022
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DOI: 10.1038/s41467-022-30532-z

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