Dual‐Metal Sites Boosting Polarization of Nitrogen Molecules for Efficient Nitrogen Photofixation

Constructing nitrogen (N2) adsorption and activation sites on semiconductors is the key to achieving efficient N2 photofixation. Herein, Mn–W dual‐metal sites on WO3 are designed toward efficient N2 photoreduction via controlled Mn doping. Impressively, the optimal 2.3% Mn‐doped WO3 (Mn‐WO3) exhibit...

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Bibliographic Details
Published in:Advanced science 2021-07, Vol.8 (13), p.n/a
Main Authors: Zhang, Yida, Hou, Tingting, Xu, Quan, Wang, Qingyu, Bai, Yu, Yang, Shaokang, Rao, Dewei, Wu, Lihui, Pan, Haibin, Chen, Jiafu, Wang, Gongming, Zhu, Junfa, Yao, Tao, Zheng, Xusheng
Format: Article
Language:English
Subjects:
Adsorption
Alternative energy sources
dual‐metal sites
manganese
Microscopy
Morphology
Nanocrystals
Nitrogen
nitrogen fixation
NMR
Nuclear magnetic resonance
Photocatalysis
polarization
Spectrum analysis
Tomography
tungsten oxides
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Summary:Constructing nitrogen (N2) adsorption and activation sites on semiconductors is the key to achieving efficient N2 photofixation. Herein, Mn–W dual‐metal sites on WO3 are designed toward efficient N2 photoreduction via controlled Mn doping. Impressively, the optimal 2.3% Mn‐doped WO3 (Mn‐WO3) exhibits a remarkable ammonia (NH3) production rate of 425 µmol gcat.−1 h−1, representing the best catalytic performance among the ever‐reported tungsten oxide‐based photocatalysts for N2 fixation. Quasi in situ synchrotron radiation X‐ray spectroscopy directly identifies that the Mn–W dual‐metal sites can enhance the polarization of the adsorbed N2, which is beneficial to the N2 activation. Further theoretical calculations reveal that the increased polarization is originated from the electron back‐donation into the antibonding orbitals of the adsorbed N2, hence lowering the reaction energy barrier toward the N2 photofixation. The concept of dual sites construction for inert molecule activation offers a powerful platform toward rational design of highly efficient catalysts for nitrogen fixation and beyond. The optimal 2.3% Mn‐doped WO3 exhibits an impressive NH3 production rate of 425 µmol gcat.−1 h−1. Further quasi in situ synchrotron radiation X‐ray spectroscopy and theoretical calculations reveal that the Mn–W dual‐metal sites can enhance the polarization of the adsorbed N2, hence lowering the reaction energy barrier toward the N2 photofixation.
ISSN:2198-3844
2198-3844
DOI:10.1002/advs.202100302