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

是否译文：

否