摘要
High yield production of phenol from hydroxylation of benzene with low energy consumption is of paramount importance,but still challenging.Herein,a new strategy,consisting of using diatomic synergistic modulation(DSM)to effectively control the separation of photo-generated carriers for an enhanced production of phenol is reported.The atomic level dispersion of Fe and Cr respectively decorated on Al based MIL-53-NH_(2)photocatalyst(Fe1/Cr:MIL-53-NH_(2))is designed,in which Cr single atoms are substituted for Al3+while Fe single atoms are coordinated by N.Notably,the Fe1/Cr:MIL-53-NH_(2)significantly boosts the photooxidation of benzene to phenol under visible light irradiation,which is much higher than those of MIL-53-NH_(2),Cr:MIL-53-NH_(2),Fe1/MIL-53-NH_(2),and Fe nanoparticles/Cr:MIL-53-NH_(2)catalysts.Theoretical and experimental results reveal that the Cr single atoms and Fe single atoms can act as electron acceptor and electron donor,respectively,during photocatalytic reaction,exhibiting a synergistic effect on the separation of the photo-generated carriers and thereby causing great enhancement on the benzene oxidation.This strategy provides new insights for rational design of advanced photocatalysts at the atomic level.
基金
the National Natural Science Foundation of China(No.21971002)
the Natural Science Foundation of Anhui Province(Nos.1908085QB45 and 2008085QB81)。