Litcius/Paper detail

Regulating Local Electron Density of Iron Single Sites by Introducing Nitrogen Vacancies for Efficient Photo‐Fenton Process

Lina Su, Pengfei Wang, Xiaoli Ma, Junhui Wang, Sihui Zhan

2021Angewandte Chemie38 citationsDOI

Abstract

Abstract 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.

Topics & Concepts

PhotocatalysisNitrogenCatalysisElectron transferAtom (system on chip)ElectronPhotochemistryMaterials scienceCarbon nitrideNitrideSpectroscopyAbsorption (acoustics)Degradation (telecommunications)Density functional theoryChemistryNanotechnologyComputational chemistryEmbedded systemQuantum mechanicsComposite materialTelecommunicationsPhysicsOrganic chemistryBiochemistryComputer scienceLayer (electronics)Advanced Photocatalysis TechniquesCatalytic Processes in Materials ScienceCopper-based nanomaterials and applications