龙冉 博士生导师  硕士生导师

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联系方式:longran@ustc.edu.cn

学位:博士

学科: 核科学与技术 、 化学

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

发布时间:2023-01-16
点击次数:
DOI码:
10.1038/s41467-022-30532-z
发表刊物:
NATURE COMMUNICATIONS
刊物所在地:
BERLIN
摘要:
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.
合写作者:
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
第一作者:
Zhang, Wenqing
通讯作者:
Long, R, Xiong, YJ
论文编号:
WOS:000798347800054
文献类型:
Article
卷号:
13
期号:
1
页面范围:
-
ISSN号:
2041-1723
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