In order to solve the problems of environment pollution and high cost in traditional process of bismuth subcarbonate preparation, a new process using ball-milling transformation method from NH4HCO3 and Bi2O3 was propo...In order to solve the problems of environment pollution and high cost in traditional process of bismuth subcarbonate preparation, a new process using ball-milling transformation method from NH4HCO3 and Bi2O3 was proposed. Additionally, the kinetics of bismuth subcarbonate preparation was studied. Effects of reaction temperature, particle size of bismuth oxide, solid-to-liquid ratio and concentrations of ammonium bicarbonate on the conversion rate of bismuth oxide were studied. The results indicate that the conversion rate of bismuth oxide significantly increased under the conditions of higher temperature, smaller particle size, higher concentration of ammonium bicarbonate and smaller solid-to-liquid ratio. The XRD and ICP-AES analyses show that the purity of product is high. The reaction kinetics with activation energy of 9.783 kJ/mol was analyzed by shrinking core model, and the whole transformation process is controlled by solid product layer diffusion. A semi-empirical kinetics equation was obtained to describe the conversion process.展开更多
A two‐step photocatalytic water splitting system,termed a“Z‐scheme system”,was achieved using Zn‐doped g‐C3N4for H2evolution and BiVO4for O2evolution with Fe2+/Fe3+as a shuttle redox mediator.H2and O2were evalua...A two‐step photocatalytic water splitting system,termed a“Z‐scheme system”,was achieved using Zn‐doped g‐C3N4for H2evolution and BiVO4for O2evolution with Fe2+/Fe3+as a shuttle redox mediator.H2and O2were evaluated simultaneously when the doping amount of zinc was10%.Moreover,Zn‐doped(10%)g‐C3N4synthesized by an impregnation method showed superior active ability to form the Z‐scheme with BiVO4than by in‐situ synthesis.X‐ray diffraction,UV‐Vis spectroscopy,scanning electron microscopy,and X‐ray photoelectron spectroscopy were used to characterize the samples.It was determined that more Zn?N bonds could be formed on the surface of g‐C3N4by impregnation,which could facilitate charge transfer.展开更多
Constructing Z-scheme heterojunction to improve the separation efficiency of photogenerated carriers of photocatalysts has gained extensive attention.In this work,we fabricated a novel Z-scheme MoO3/Bi2O4 heterojuncti...Constructing Z-scheme heterojunction to improve the separation efficiency of photogenerated carriers of photocatalysts has gained extensive attention.In this work,we fabricated a novel Z-scheme MoO3/Bi2O4 heterojunction photocatalyst by a hydrothermal method.XPS analysis results indicated that strong interaction between MoO3 and Bi2O4 is generated,which contributes to charge transfer and separation of the photogenerated carriers.This was confirmed by photoluminescence(PL)and electrochemical impedance spectroscopy(EIS)tests.The photocatalytic performance of the as-synthesized photocatalysts was evaluated by degrading rhodamine B(RhB)in aqueous solution under visible light irradiation,showing that 15%MoO3/Bi2O4(15-MB)composite exhibited the highest photocatalytic activity,which is 2 times higher than that of Bi2O4.Besides,the heterojunction photocatalyst can keep good photocatalytic activity and stability after five recycles.Trapping experiments demonstrated that the dominant active radicals in photocatalytic reactions are superoxide radical( O2-)and holes(h+),indicating that the 15-MB composite is a Z-scheme photocatalyst.Finally,the mechanism of the Z-scheme MoO3/Bi2O4 composite for photo-degrading RhB in aqueous solution is proposed.This work provides a promising strategy for designing Bi-based Z-scheme heterojunction photocatalysts for highly efficient removal of environmental pollutants.展开更多
In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) ...In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) reduction was studied under visible light.The as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites show a superior activity for photocatalytic CO_(2) reduction to produce CH4 and CO,with an optimum activity achieved over 0.5 Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6).The obvious superior activity observed over Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites as compared with bare Cs_(2)AgBiBr_(6) and bare Bi_(2)WO_(6) as well as a mechanical mixture of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) can be owe to the fabrication of an efficient S-scheme heterojunction,which accelerates the separation of the photogenerated charge carriers in Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) without sacrificing the high redox capability of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6).This work demonstrates that the coupling of two photocatalytic materials with staggered band alignment to form an S-scheme heterojunction is an effective strategy to develop efficient photocatalytic systems and also highlights the promising role of using lead free perovskites in photocatalysis.展开更多
The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/...The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi(CN/BMO/Bi)hollow microsphere was successfully fabricated through solvothermal and in situ reduction methods.The results revealed that the optimal ternary 0.4 CN/BMO/9 Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B(RhB)degradation with nine times that of pure BMO.The DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4 CN/BMO/9 Bi is a z-scheme structure.Quenching experiments also provided solid evidence that the·O^2-(at-0.33 eV)is the main species during dye degradation,and the conduction band of g-C3N4 is only the reaction site,demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2 MoO 6/Bi is through an indirect z-scheme structure.Thus,the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping,resulting in better optical absorption ability and a lower combination rate of photogenerated charge carriers.The findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.展开更多
Bismuth selenide(Bi_(2)Se_(3))is an attractive visible-light-responsive semiconductor that can absorb a full range of visible and near-infrared light.However,its poor redox capacity and rapid carrier recombination lim...Bismuth selenide(Bi_(2)Se_(3))is an attractive visible-light-responsive semiconductor that can absorb a full range of visible and near-infrared light.However,its poor redox capacity and rapid carrier recombination limit its application in photocatalytic oxidation.In this study,we adopted Bi_(2)Se_(3)as the couple part of graphitic carbon nitride(g-C_(3)N_(4))to construct a Bi_(2)Se_(3)/g-C_(3)N_(4)composite photocatalyst.Through in situ fabrication,the self-developed Bi2O3/g-C_(3)N_(4)precursor was transformed into a Bi_(2)Se_(3)/g-C_(3)N_(4)heterojunction.The as-prepared Bi_(2)Se_(3)/g-C_(3)N_(4)composite exhibited much higher visible-light-driven photocatalytic activity than pristine Bi_(2)Se_(3)and g-C_(3)N_(4)in the removal of phenol.The enhanced photocatalytic activity was ascribed to the S-scheme configuration of Bi_(2)Se_(3)/g-C_(3)N_(4);this was confirmed by the energy-level shift,photoluminescence analysis,computational structure study,and reactive-radical testing.In the S-scheme heterojunction,photo-excited electrons in the conduction band of g-C_(3)N_(4)migrate to the valence band of Bi_(2)Se_(3)and combine with the excited holes therein.By consuming less reactive carriers,the S-scheme heterojunction can not only effectively promote charge separation,but also preserve more reactive photo-generated carriers.This property enhances the photocatalytic activity.展开更多
基金Project(50774099)supported by the National Natural Science Foundation of China
文摘In order to solve the problems of environment pollution and high cost in traditional process of bismuth subcarbonate preparation, a new process using ball-milling transformation method from NH4HCO3 and Bi2O3 was proposed. Additionally, the kinetics of bismuth subcarbonate preparation was studied. Effects of reaction temperature, particle size of bismuth oxide, solid-to-liquid ratio and concentrations of ammonium bicarbonate on the conversion rate of bismuth oxide were studied. The results indicate that the conversion rate of bismuth oxide significantly increased under the conditions of higher temperature, smaller particle size, higher concentration of ammonium bicarbonate and smaller solid-to-liquid ratio. The XRD and ICP-AES analyses show that the purity of product is high. The reaction kinetics with activation energy of 9.783 kJ/mol was analyzed by shrinking core model, and the whole transformation process is controlled by solid product layer diffusion. A semi-empirical kinetics equation was obtained to describe the conversion process.
基金supported by the National Natural Science Foundation of China (21773153)~~
文摘A two‐step photocatalytic water splitting system,termed a“Z‐scheme system”,was achieved using Zn‐doped g‐C3N4for H2evolution and BiVO4for O2evolution with Fe2+/Fe3+as a shuttle redox mediator.H2and O2were evaluated simultaneously when the doping amount of zinc was10%.Moreover,Zn‐doped(10%)g‐C3N4synthesized by an impregnation method showed superior active ability to form the Z‐scheme with BiVO4than by in‐situ synthesis.X‐ray diffraction,UV‐Vis spectroscopy,scanning electron microscopy,and X‐ray photoelectron spectroscopy were used to characterize the samples.It was determined that more Zn?N bonds could be formed on the surface of g‐C3N4by impregnation,which could facilitate charge transfer.
基金supported by the Natural Science Foundation of Hubei Province(2016CFA078)the National Natural Science Foundation of China(51472194)~~
文摘Constructing Z-scheme heterojunction to improve the separation efficiency of photogenerated carriers of photocatalysts has gained extensive attention.In this work,we fabricated a novel Z-scheme MoO3/Bi2O4 heterojunction photocatalyst by a hydrothermal method.XPS analysis results indicated that strong interaction between MoO3 and Bi2O4 is generated,which contributes to charge transfer and separation of the photogenerated carriers.This was confirmed by photoluminescence(PL)and electrochemical impedance spectroscopy(EIS)tests.The photocatalytic performance of the as-synthesized photocatalysts was evaluated by degrading rhodamine B(RhB)in aqueous solution under visible light irradiation,showing that 15%MoO3/Bi2O4(15-MB)composite exhibited the highest photocatalytic activity,which is 2 times higher than that of Bi2O4.Besides,the heterojunction photocatalyst can keep good photocatalytic activity and stability after five recycles.Trapping experiments demonstrated that the dominant active radicals in photocatalytic reactions are superoxide radical( O2-)and holes(h+),indicating that the 15-MB composite is a Z-scheme photocatalyst.Finally,the mechanism of the Z-scheme MoO3/Bi2O4 composite for photo-degrading RhB in aqueous solution is proposed.This work provides a promising strategy for designing Bi-based Z-scheme heterojunction photocatalysts for highly efficient removal of environmental pollutants.
文摘In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) reduction was studied under visible light.The as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites show a superior activity for photocatalytic CO_(2) reduction to produce CH4 and CO,with an optimum activity achieved over 0.5 Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6).The obvious superior activity observed over Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites as compared with bare Cs_(2)AgBiBr_(6) and bare Bi_(2)WO_(6) as well as a mechanical mixture of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) can be owe to the fabrication of an efficient S-scheme heterojunction,which accelerates the separation of the photogenerated charge carriers in Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) without sacrificing the high redox capability of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6).This work demonstrates that the coupling of two photocatalytic materials with staggered band alignment to form an S-scheme heterojunction is an effective strategy to develop efficient photocatalytic systems and also highlights the promising role of using lead free perovskites in photocatalysis.
基金financially supported by the Science Foundation of China University of Petroleum,Beijing(2462017YJRC048,2462018BJC005)the National Natural Science Foundation of China(51802351)~~
文摘The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi(CN/BMO/Bi)hollow microsphere was successfully fabricated through solvothermal and in situ reduction methods.The results revealed that the optimal ternary 0.4 CN/BMO/9 Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B(RhB)degradation with nine times that of pure BMO.The DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4 CN/BMO/9 Bi is a z-scheme structure.Quenching experiments also provided solid evidence that the·O^2-(at-0.33 eV)is the main species during dye degradation,and the conduction band of g-C3N4 is only the reaction site,demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2 MoO 6/Bi is through an indirect z-scheme structure.Thus,the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping,resulting in better optical absorption ability and a lower combination rate of photogenerated charge carriers.The findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.
文摘Bismuth selenide(Bi_(2)Se_(3))is an attractive visible-light-responsive semiconductor that can absorb a full range of visible and near-infrared light.However,its poor redox capacity and rapid carrier recombination limit its application in photocatalytic oxidation.In this study,we adopted Bi_(2)Se_(3)as the couple part of graphitic carbon nitride(g-C_(3)N_(4))to construct a Bi_(2)Se_(3)/g-C_(3)N_(4)composite photocatalyst.Through in situ fabrication,the self-developed Bi2O3/g-C_(3)N_(4)precursor was transformed into a Bi_(2)Se_(3)/g-C_(3)N_(4)heterojunction.The as-prepared Bi_(2)Se_(3)/g-C_(3)N_(4)composite exhibited much higher visible-light-driven photocatalytic activity than pristine Bi_(2)Se_(3)and g-C_(3)N_(4)in the removal of phenol.The enhanced photocatalytic activity was ascribed to the S-scheme configuration of Bi_(2)Se_(3)/g-C_(3)N_(4);this was confirmed by the energy-level shift,photoluminescence analysis,computational structure study,and reactive-radical testing.In the S-scheme heterojunction,photo-excited electrons in the conduction band of g-C_(3)N_(4)migrate to the valence band of Bi_(2)Se_(3)and combine with the excited holes therein.By consuming less reactive carriers,the S-scheme heterojunction can not only effectively promote charge separation,but also preserve more reactive photo-generated carriers.This property enhances the photocatalytic activity.