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

DOI number:10.1038/s41467-022-30532-z

Journal:NATURE COMMUNICATIONS

Place of Publication:BERLIN

Abstract:Photocatalytic nonoxidative coupling of methane (NOCM) emerges as an appealing approach for the production of value-added C2 + hydrocarbons and hydrogen. Here the authors propose a heteroatom engineering strategy to prepare Pd single atoms loaded TiO2 for active and selective photocatalytic NOCM. 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-O-4 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 H-2 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.

Co-author:Zhang, Wenqing, Fu, Cenfeng, Low, Jingxiang, Duan, Delong, Ma, Jun, Jiang, Wenbin, Chen, Yihong, Hengjie, Qi, Zeming, Long, Ran, Yao, Yingfang, Li, Xiaobao, Zhang, Hui, Liu, Zhi, Yang, Jinlong, Zou, Zhigang, Xiong, Yujie

First Author:Zhang, Wenqing

Correspondence Author:Long, R, Xiong, YJ

Document Code:WOS:000798347800054

Document Type:Article

Volume:13

Issue:1

Page Number:-

ISSN No.:2041-1723

Translation or Not:no