Hole/electron separation and charge transfer are the key processes for enhancing the visible-light photocatalysis performance of heterogeneous photocatalytic systems.To better utilize and understand these effects,bina...Hole/electron separation and charge transfer are the key processes for enhancing the visible-light photocatalysis performance of heterogeneous photocatalytic systems.To better utilize and understand these effects,binary Ag3PO4/Ag2MoO4 hybrid materials were fabricated by a facile solution-phase reaction and characterized systematically by X-ray diffraction(XRD),energy-dispersive spectroscopy,Fourier transform infrared spectroscopy,Raman spectroscopy,field-emission scanning electron microscopy and ultraviolet-visible diffuse-reflectance spectroscopy.Under visible-light illumination,a heterogeneous Ag3PO4/Ag/Ag2MoO4 photocatalyst was constructed and demonstrated enhanced photocatalytic activity and photostability compared with pristine Ag3PO4toward the remediation of the organic dye rhodamine B.The Ag3PO4/Ag2MoO4 hybrid catalyst with8%mole fraction of Ag2MoO4 exhibited the highest photocatalytic activity toward the removal of typical dye molecules,including methyl orange,methylene blue and phenol aqueous solution.Moreover,the mechanism of the photocatalytic enhancement was investigated via hole- and radical-trapping experiments,photocurrent measurements,electrochemical impedance spectroscopy and XRD measurements.The XRD analysis revealed that metallic Ag nanoparticles formed initially on the surface of the Ag3PO4/Ag2MoO4 composites under visible-light illumination,leading to the generation of a Ag3PO4/Ag/Ag2MoO4 Z-scheme tandem photocatalytic system.The enhanced photocatalytic activity and stability were attributed to the formation of the Ag3PO4/Ag/Ag2MoO4Z-scheme heterojunction and surface plasmon resonance of photo-reduced Ag nanoparticles on the surface.Finally,a plasmonic Z-scheme photocatalytic mechanism was proposed.This work may provide new insights into the design and preparation of advanced visible-light photocatalytic materials and facilitate their practical application in environmental issues.展开更多
LaTaON_(2)is an attractive visible-light-active photocatalyst for water splitting due to its broad visible light absorption as far as 650 nm and proper band edge positions.Notwithstanding these promising properties,La...LaTaON_(2)is an attractive visible-light-active photocatalyst for water splitting due to its broad visible light absorption as far as 650 nm and proper band edge positions.Notwithstanding these promising properties,LaTaON_(2)generally exhibits poor photocatalytic activity because of its high defect concentration that severely hinders charge separation.Here,LaTaON_(2)has been modified by doping Al into the Ta sublattice,i.e.,LaTa_(1−x)Al_(x)O_(1+y)N_(2−y)(0≤x≤0.20).Al doping not only inhibits the defect concentration and increases surface hydrophilicity but also maintains the desired visible light absorption of LaTaON_(2).These important modifications substantially ameliorate the charge separation conditions within LaTaON_(2)and are responsible for a much enhanced photocatalytic performance for water redox reactions under visible light illumination.Under optimal conditions,the Al-doped LaTaON_(2)delivers an apparent quantum efficiency of 1.17%at 420±20 nm for water oxidation into O_(2),outperforming most LaTaON_(2)-based photocatalysts.These findings highlight Al as a useful dopant to open up the photocatalytic potential of metal oxynitrides whose activity is often undermined by a high defect concentration.展开更多
基金supported by the National Natural Science Foundation of China (51672113, 51302112)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology, 2016-KF-10)~~
文摘Hole/electron separation and charge transfer are the key processes for enhancing the visible-light photocatalysis performance of heterogeneous photocatalytic systems.To better utilize and understand these effects,binary Ag3PO4/Ag2MoO4 hybrid materials were fabricated by a facile solution-phase reaction and characterized systematically by X-ray diffraction(XRD),energy-dispersive spectroscopy,Fourier transform infrared spectroscopy,Raman spectroscopy,field-emission scanning electron microscopy and ultraviolet-visible diffuse-reflectance spectroscopy.Under visible-light illumination,a heterogeneous Ag3PO4/Ag/Ag2MoO4 photocatalyst was constructed and demonstrated enhanced photocatalytic activity and photostability compared with pristine Ag3PO4toward the remediation of the organic dye rhodamine B.The Ag3PO4/Ag2MoO4 hybrid catalyst with8%mole fraction of Ag2MoO4 exhibited the highest photocatalytic activity toward the removal of typical dye molecules,including methyl orange,methylene blue and phenol aqueous solution.Moreover,the mechanism of the photocatalytic enhancement was investigated via hole- and radical-trapping experiments,photocurrent measurements,electrochemical impedance spectroscopy and XRD measurements.The XRD analysis revealed that metallic Ag nanoparticles formed initially on the surface of the Ag3PO4/Ag2MoO4 composites under visible-light illumination,leading to the generation of a Ag3PO4/Ag/Ag2MoO4 Z-scheme tandem photocatalytic system.The enhanced photocatalytic activity and stability were attributed to the formation of the Ag3PO4/Ag/Ag2MoO4Z-scheme heterojunction and surface plasmon resonance of photo-reduced Ag nanoparticles on the surface.Finally,a plasmonic Z-scheme photocatalytic mechanism was proposed.This work may provide new insights into the design and preparation of advanced visible-light photocatalytic materials and facilitate their practical application in environmental issues.
基金the National Natural Science Foundation of China(51972233 and 52172225)the Natural Science Foundation of Shanghai(19ZR1459200)+1 种基金the Science and Technology Commission of Shanghai Municipality(19DZ2271500)the Fundamental Research Funds for the Central Universities.
文摘LaTaON_(2)is an attractive visible-light-active photocatalyst for water splitting due to its broad visible light absorption as far as 650 nm and proper band edge positions.Notwithstanding these promising properties,LaTaON_(2)generally exhibits poor photocatalytic activity because of its high defect concentration that severely hinders charge separation.Here,LaTaON_(2)has been modified by doping Al into the Ta sublattice,i.e.,LaTa_(1−x)Al_(x)O_(1+y)N_(2−y)(0≤x≤0.20).Al doping not only inhibits the defect concentration and increases surface hydrophilicity but also maintains the desired visible light absorption of LaTaON_(2).These important modifications substantially ameliorate the charge separation conditions within LaTaON_(2)and are responsible for a much enhanced photocatalytic performance for water redox reactions under visible light illumination.Under optimal conditions,the Al-doped LaTaON_(2)delivers an apparent quantum efficiency of 1.17%at 420±20 nm for water oxidation into O_(2),outperforming most LaTaON_(2)-based photocatalysts.These findings highlight Al as a useful dopant to open up the photocatalytic potential of metal oxynitrides whose activity is often undermined by a high defect concentration.