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

摘要

The activity of heterogeneous photocatalytic H2O2 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 H2O2 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 H2O2 conversion efficiency. Therefore, the optimized single atom catalyst exhibiting a higher ciprofloxacin degradation activity, which was up to 18 times that of pristine CN.