Although different NbO_(x) units are present in Nb_(2)O_(5)‐based catalysts,the correlations between these structures and activity remain unclear,which considerably hinders the further development of Nb_(2)O_(5) phot...Although different NbO_(x) units are present in Nb_(2)O_(5)‐based catalysts,the correlations between these structures and activity remain unclear,which considerably hinders the further development of Nb_(2)O_(5) photocatalysis.Herein,we utilized N‐hydroxyphthalimide(NHPI)as the probe molecule to distinguish the role of different NbO_(x) units in the activation of C–H bond under visible light irradia‐tion.With the addition of NHPI,Nb_(2)O_(5) catalysts with highly disordered NbO_(6) units exhibited higher activities than that with slightly disordered NbO_(6) units(419‒495 vs.82μmol·g^(-1)·h^(-1))in photocata‐lytic selective oxidation of ethylbenzene.Revealed by Raman spectra,electron paramagnetic reso‐nance spectra,and transmission‐electron‐microscopy images,highly disordered NbO_(6) units were confirmed to act as the active sites for the transfer of photogenerated electrons from NHPI,pro‐moting the generation of phthalimide‐N‐oxyl(PINO)radicals for the enhanced conversion of ethylbenzene under visible light irradiation.This study provides guidance on the role of local NbO_(x) units in Nb_(2)O_(5) photocatalysis.展开更多
Nonylphenol(NP)residues,as a typical endocrine disrupting chemical(EDC),frequently exist in sewage,surface water,groundwater and even drinking water,which poses a serious threat to human health due to its bioaccumulat...Nonylphenol(NP)residues,as a typical endocrine disrupting chemical(EDC),frequently exist in sewage,surface water,groundwater and even drinking water,which poses a serious threat to human health due to its bioaccumulation.In order to remove NP,a series of MIL-100(Fe)/Zn Fe_(2)O_(4)/flake-like porous carbon nitride(MIL/ZC)was synthesized through in-situ synthesis at room temperature.High performance of ternary MIL/ZC is used to degrade NP under visible light irradiation.The results show that 30MIL/ZC2(20 wt.%Zn Fe_(2)O_(4))ternary composite had the best photocatalytic activity(99.84%)when the dosage was 30 mg.Further mechanism analysis shows that the excellent photocatalytic activity of 30MIL/ZC2could be ascribed to the double charge transfer process between flake-like porous carbon nitride(PCN)and other catalysts in the ternary heterojunction,and the separation of photogenerated electron-hole pairs was more effective.In addition,the 30MIL/ZC2 also showed high stability after five cycles of the photodegradation reaction.Furthermore,the active substance(·O_(2)^(-))was considered to be the main active substance in the NP degradation process.Based on the research results,the possible photocatalytic reaction mechanism of 30MIL/ZC2ternary composite was proposed and discussed in detail.展开更多
文摘Although different NbO_(x) units are present in Nb_(2)O_(5)‐based catalysts,the correlations between these structures and activity remain unclear,which considerably hinders the further development of Nb_(2)O_(5) photocatalysis.Herein,we utilized N‐hydroxyphthalimide(NHPI)as the probe molecule to distinguish the role of different NbO_(x) units in the activation of C–H bond under visible light irradia‐tion.With the addition of NHPI,Nb_(2)O_(5) catalysts with highly disordered NbO_(6) units exhibited higher activities than that with slightly disordered NbO_(6) units(419‒495 vs.82μmol·g^(-1)·h^(-1))in photocata‐lytic selective oxidation of ethylbenzene.Revealed by Raman spectra,electron paramagnetic reso‐nance spectra,and transmission‐electron‐microscopy images,highly disordered NbO_(6) units were confirmed to act as the active sites for the transfer of photogenerated electrons from NHPI,pro‐moting the generation of phthalimide‐N‐oxyl(PINO)radicals for the enhanced conversion of ethylbenzene under visible light irradiation.This study provides guidance on the role of local NbO_(x) units in Nb_(2)O_(5) photocatalysis.
基金supported by the National Natural Science Foundation of China(No.21477050)the International Scientific and Technological Cooperation in Changzhou(No.CZ20140017)+2 种基金Postgraduate Research Innovation Project of Jiangsu Province(Nos.KYCX20_2561,KYCX20_2598)the Jiangsu Planned Projects for Postdoctoral Research Funds(No.2019K112)the Jiangsu Province subsidizes the recruitment of postdoctoral personnel(No.2019Z143)。
文摘Nonylphenol(NP)residues,as a typical endocrine disrupting chemical(EDC),frequently exist in sewage,surface water,groundwater and even drinking water,which poses a serious threat to human health due to its bioaccumulation.In order to remove NP,a series of MIL-100(Fe)/Zn Fe_(2)O_(4)/flake-like porous carbon nitride(MIL/ZC)was synthesized through in-situ synthesis at room temperature.High performance of ternary MIL/ZC is used to degrade NP under visible light irradiation.The results show that 30MIL/ZC2(20 wt.%Zn Fe_(2)O_(4))ternary composite had the best photocatalytic activity(99.84%)when the dosage was 30 mg.Further mechanism analysis shows that the excellent photocatalytic activity of 30MIL/ZC2could be ascribed to the double charge transfer process between flake-like porous carbon nitride(PCN)and other catalysts in the ternary heterojunction,and the separation of photogenerated electron-hole pairs was more effective.In addition,the 30MIL/ZC2 also showed high stability after five cycles of the photodegradation reaction.Furthermore,the active substance(·O_(2)^(-))was considered to be the main active substance in the NP degradation process.Based on the research results,the possible photocatalytic reaction mechanism of 30MIL/ZC2ternary composite was proposed and discussed in detail.