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Regulating Local Electron Density of Iron Single Sites by Introducing Nitrogen Vacancies for Efficient Photo‐Fenton Process
Author(s) -
Su Lina,
Wang Pengfei,
Ma Xiaoli,
Wang Junhui,
Zhan Sihui
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202108937
Subject(s) - photocatalysis , nitrogen , catalysis , electron , atom (system on chip) , electron transfer , materials science , photochemistry , nitride , degradation (telecommunications) , carbon nitride , spectroscopy , density functional theory , absorption (acoustics) , atomic physics , chemistry , nanotechnology , computational chemistry , physics , telecommunications , biochemistry , organic chemistry , layer (electronics) , quantum mechanics , computer science , embedded system , composite material
The activity of heterogeneous photocatalytic H 2 O 2 activation in Fenton‐like processes is closely related to the local electron density of reaction centre atoms. However, the recombination of electron‐hole pairs arising from random charge transfer greatly restricts the oriented electron delivery to active center. Here we show a defect engineered iron single atom photocatalyst (Fe 1 ‐N v /CN, single Fe atoms dispersed on carbon nitride with abundant nitrogen vacancies) for the activation of H 2 O 2 under visible light irradiation. Based on DFT calculations and transient absorption spectroscopy results, the engineered nitrogen vacancies serve as the electron trap sites, which can directionally drive the electrons to concentrate on Fe atoms. The formation of highly concentrated electrons density at Fe sites significantly improves the H 2 O 2 conversion efficiency. Therefore, the optimized single atom catalyst exhibiting a higher ciprofloxacin degradation activity, which was up to 18 times that of pristine CN.