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Non‐oxidative Coupling of Methane: N‐type Doping of Niobium Single Atoms in TiO 2 –SiO 2 Induces Electron Localization
Author(s) -
Chen Ziyu,
Wu Shiqun,
Ma Jiayu,
Mine Shinya,
Toyao Takashi,
Matsuoka Masaya,
Wang Lingzhi,
Zhang Jinlong
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202016420
Subject(s) - dopant , doping , methane , materials science , desorption , atom (system on chip) , analytical chemistry (journal) , inorganic chemistry , adsorption , chemistry , organic chemistry , optoelectronics , computer science , embedded system
Photodriven nonoxidative coupling of CH 4 (NOCM) is an attractive potential way to use abundant methane resources. Herein, an n‐type doped photocatalyst for NOCM is created by doping single‐atom Nb into hierarchical porous TiO 2 –SiO 2 (TS) microarray, which exhibits a high conversion rate of 3.57 μmol g −1 h −1 with good recyclability. The Nb dopant replaces the 6‐coordinated titanium on the (1 0 1) plane and forms shallow electron‐trapped surface polarons along [0 1 0] direction and the comparison of different models proves that the electron localization caused by the n‐type doping is beneficial to both methane activation and ethane desorption. The positive effect of n‐type dopant on CH 4 conversion is further verified on Mo‐, W‐ and Ta‐doped composites. In contrast, the doping of p‐type dopant (Ga, Cu, Fe) shows a less active influence.