A simple calcination method was employed to prepare a Z-scheme N-doped K4Nb6O17/g-C3N4(KCN)heterojunction photocatalyst,in which the electronic structure of K4Nb6O17 was regulated by N-doping,and g-C3N4 was formed bot...A simple calcination method was employed to prepare a Z-scheme N-doped K4Nb6O17/g-C3N4(KCN)heterojunction photocatalyst,in which the electronic structure of K4Nb6O17 was regulated by N-doping,and g-C3N4 was formed both on the surface and within the interlayer spaces of K4Nb6O17.The KCN composite showed profoundly improved photocatalytic activity for both H2 generation and RhB degradation compared to its counterparts.This improved performance was attributed to the synergistic effects of N-doping,which broadened its light harvesting ability,and heterojunction formation,which increased the charge separation rate.The relatively low BET specific surface area of the KCN composite had little effect on its photocatalytic activity.Based on ESR spectroscopy studies,•O2^−,•OH,and h^+are the main active species in the photocatalytic degradation of RhB.Thus,it is reasonable to propose a Z-scheme photocatalytic mechanism over the KCN composite,which exhibits the dual advantages of efficient charge separation and high redox ability.Our work provides a simple approach for constructing large-scale Z-scheme heterojunction photocatalysts with high photocatalytic performance.展开更多
The fabrication of S-scheme heterojunctions with fast charge transfer and good interface contacts,such as intermolecularπ–πinteractions,is a promising approach to improve photocatalytic performance.A unique two-dim...The fabrication of S-scheme heterojunctions with fast charge transfer and good interface contacts,such as intermolecularπ–πinteractions,is a promising approach to improve photocatalytic performance.A unique two-dimensional/two-dimensional(2D/2D)S-scheme heterojunction containing TpPa-1-COF/g-C_(3)N_(4) nanosheets(denoted as TPCNNS)was developed.The established maximum interfacial interaction between TpPa-1-COF NS and g-C_(3)N_(4) NS may result in aπ–πconjugated heterointerface.Furthermore,the difference in the work functions of TpPa-1-COF and g-C_(3)N_(4) results in a large Fermi level gap,leading to upward/downward band edge bending.The spontaneous interfacial charge transfer from g-C_(3)N_(4) to TpPa-1-COF at theπ–πconjugated interface area results in the presence of a built-in electric field,according to the charge density difference analysis based on density functional theory calculations.Such an enhanced built-in electric field can efficiently drive directional charge migration via the S-scheme mechanism,which enhances charge separation and utilization.Thus,an approximately 2.8 and 5.6 times increase in the photocatalytic hydrogen evolution rate was recorded in TPCNNS-2(1153μmol g^(-1) h^(-1))compared to pristine TpPa-1-COF and g-C_(3)N_(4) NS,respectively,under visible light irradiation.Overall,this work opens new avenues in the fabrication of 2D/2Dπ–πconjugated S-scheme heterojunction photocatalysts with highly efficient hydrogen evolution performance.展开更多
We have investigated the adsorption of nine different adatoms on the(111)and(100)surfaces of Iridium(Ir)using first principles density functional theory.The study explores surface functionalization of Ir which would p...We have investigated the adsorption of nine different adatoms on the(111)and(100)surfaces of Iridium(Ir)using first principles density functional theory.The study explores surface functionalization of Ir which would provide important information for further study of its functionality in catalysis and other surface applications.The adsorption energy,stable geometry,density of states and magnetic moment are some of the physical quantities of our interest.The study reveals that the three-/four-fold hollow site is energetically the most favorable adsorption site on the(111)/(100)surface of Ir.The investigation on a wide range of coverages(from 0.04 to 1 monolayer)reveals the strong coverage dependence of adsorption energy of the adsorbate atoms.The adsorption energy is found to increase as the coverage increases,implying a repulsive interaction between the adsorbates.Strong hybridization between the adsorbates and the substrate electronic states is revealed to impact the adsorption,while the magnetic moment of the adsorbates is found to be suppressed.The Bader analysis reveals significant amount of charge transfers between the adsorbate atoms and the substrate.The binding of adsorbate atoms on the(100)surface is observed to be moderately stronger as compared to that on the(111)surface.展开更多
Tin dioxide (SnO2) has attracted broad interest due to its particular gas-sensor property. Nano- or atom-scale SnO2 material has always been the aim in order to ultimately improve the sensitivity. However, until now, ...Tin dioxide (SnO2) has attracted broad interest due to its particular gas-sensor property. Nano- or atom-scale SnO2 material has always been the aim in order to ultimately improve the sensitivity. However, until now, it remains difficult to synthesize SnO2 nanoclusters by using traditional methods. In the present work, we have achieved the preparation of SnO2 nanoclusters by using the cluster beam deposition technique. The obtained nanoclusters were well characterized by high resolution transmission electron microscope HR-TEM. Results indicated the formation of the well-dispersed SnO2 nanoclusters with uniform size distribution (5-7 nm). Furthermore, an obvious metal insulator transition was observed by gating with ionic liquid. Combined with theory calculation, the corresponding mechanism was systematically analyzed from oxygen vacancy induced electron doping.展开更多
文摘A simple calcination method was employed to prepare a Z-scheme N-doped K4Nb6O17/g-C3N4(KCN)heterojunction photocatalyst,in which the electronic structure of K4Nb6O17 was regulated by N-doping,and g-C3N4 was formed both on the surface and within the interlayer spaces of K4Nb6O17.The KCN composite showed profoundly improved photocatalytic activity for both H2 generation and RhB degradation compared to its counterparts.This improved performance was attributed to the synergistic effects of N-doping,which broadened its light harvesting ability,and heterojunction formation,which increased the charge separation rate.The relatively low BET specific surface area of the KCN composite had little effect on its photocatalytic activity.Based on ESR spectroscopy studies,•O2^−,•OH,and h^+are the main active species in the photocatalytic degradation of RhB.Thus,it is reasonable to propose a Z-scheme photocatalytic mechanism over the KCN composite,which exhibits the dual advantages of efficient charge separation and high redox ability.Our work provides a simple approach for constructing large-scale Z-scheme heterojunction photocatalysts with high photocatalytic performance.
文摘The fabrication of S-scheme heterojunctions with fast charge transfer and good interface contacts,such as intermolecularπ–πinteractions,is a promising approach to improve photocatalytic performance.A unique two-dimensional/two-dimensional(2D/2D)S-scheme heterojunction containing TpPa-1-COF/g-C_(3)N_(4) nanosheets(denoted as TPCNNS)was developed.The established maximum interfacial interaction between TpPa-1-COF NS and g-C_(3)N_(4) NS may result in aπ–πconjugated heterointerface.Furthermore,the difference in the work functions of TpPa-1-COF and g-C_(3)N_(4) results in a large Fermi level gap,leading to upward/downward band edge bending.The spontaneous interfacial charge transfer from g-C_(3)N_(4) to TpPa-1-COF at theπ–πconjugated interface area results in the presence of a built-in electric field,according to the charge density difference analysis based on density functional theory calculations.Such an enhanced built-in electric field can efficiently drive directional charge migration via the S-scheme mechanism,which enhances charge separation and utilization.Thus,an approximately 2.8 and 5.6 times increase in the photocatalytic hydrogen evolution rate was recorded in TPCNNS-2(1153μmol g^(-1) h^(-1))compared to pristine TpPa-1-COF and g-C_(3)N_(4) NS,respectively,under visible light irradiation.Overall,this work opens new avenues in the fabrication of 2D/2Dπ–πconjugated S-scheme heterojunction photocatalysts with highly efficient hydrogen evolution performance.
基金supported by the National Natural Science Foundation of China(No.11750110415,No.11474246,and No.11774178)the Natural Science Foundation of Jiangsu Province(BK20160061)。
文摘We have investigated the adsorption of nine different adatoms on the(111)and(100)surfaces of Iridium(Ir)using first principles density functional theory.The study explores surface functionalization of Ir which would provide important information for further study of its functionality in catalysis and other surface applications.The adsorption energy,stable geometry,density of states and magnetic moment are some of the physical quantities of our interest.The study reveals that the three-/four-fold hollow site is energetically the most favorable adsorption site on the(111)/(100)surface of Ir.The investigation on a wide range of coverages(from 0.04 to 1 monolayer)reveals the strong coverage dependence of adsorption energy of the adsorbate atoms.The adsorption energy is found to increase as the coverage increases,implying a repulsive interaction between the adsorbates.Strong hybridization between the adsorbates and the substrate electronic states is revealed to impact the adsorption,while the magnetic moment of the adsorbates is found to be suppressed.The Bader analysis reveals significant amount of charge transfers between the adsorbate atoms and the substrate.The binding of adsorbate atoms on the(100)surface is observed to be moderately stronger as compared to that on the(111)surface.
基金supported by the National Natural Science Foundation of China(No.11704325,No.11604288,and No.11774178)the Natural Science Foundation of Jiangsu Province(BK20170473,BK20160061)the Joint Open Fund of Jiangsu Collaborative Innovation Center for Ecological Building Material and Environmental Protection Equipment and Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province(JH201843)
文摘Tin dioxide (SnO2) has attracted broad interest due to its particular gas-sensor property. Nano- or atom-scale SnO2 material has always been the aim in order to ultimately improve the sensitivity. However, until now, it remains difficult to synthesize SnO2 nanoclusters by using traditional methods. In the present work, we have achieved the preparation of SnO2 nanoclusters by using the cluster beam deposition technique. The obtained nanoclusters were well characterized by high resolution transmission electron microscope HR-TEM. Results indicated the formation of the well-dispersed SnO2 nanoclusters with uniform size distribution (5-7 nm). Furthermore, an obvious metal insulator transition was observed by gating with ionic liquid. Combined with theory calculation, the corresponding mechanism was systematically analyzed from oxygen vacancy induced electron doping.