光催化
杂原子
选择性
材料科学
甲烷
氢
光化学
价(化学)
石墨烯
耐久性
制氢
兴奋剂
化学
催化作用
化学工程
纳米技术
有机化学
光电子学
复合材料
戒指(化学)
工程类
作者
Wenqing Zhang,Cen‐Feng Fu,Jingxiang Low,Delong Duan,Jun Ma,Wenbin Jiang,Yihong Chen,Hengjie Liu,Zeming Qi,Ran Long,Yingfang Yao,Xiaobao Li,Hui Zhang,Zhi Li,Jinlong Yang,Zhigang Zou,Yujie Xiong
标识
DOI:10.1038/s41467-022-30532-z
摘要
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.
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