Designing defect-engineered semiconductor heterojunctions can effectively promote the charge carrier separation.Herein,novel ceria(CeO2) quantum dots(QDs) decorated sulfur-doped carbon nitride nanotubes(SCN NTs) were ...Designing defect-engineered semiconductor heterojunctions can effectively promote the charge carrier separation.Herein,novel ceria(CeO2) quantum dots(QDs) decorated sulfur-doped carbon nitride nanotubes(SCN NTs) were synthesized via a thermal polycondensation coupled in situ depositionprecipitation method without use of template or surfactant.The structure and morphology studies indicate that ultrafine CeO2 QDs are well distributed inside and outside of SCN NTs offering highly dispersed active sites and a large contact interface between two components.This leads to the promoted formation of rich Ce^(3+) ion and oxygen vacancies as confirmed by XPS.The photocatalytic performance can be facilely modulated by the content of CeO2 QDs introduced in SCN matrix while bare CeO2 does not show activity of hydrogen production.The optimal catalyst with 10% of CeO2 loading yields a hydrogen evolution rate of 2923.8 μmol h-1 g-1 under visible light,remarkably higher than that of bare SCN and their physical mixtures.Further studies reveal that the abundant surface defects and the created 0 D/1 D junctions play a critical role in improving the separation and transfer of charge carriers,leading to superior solar hydrogen production and good stability.展开更多
Sodium-doped carbon nitride nanotubes (Nax-CNNTs) were prepared by a green and simple two-step method and applied in photocatalytic water splitting for the first time. Transmission electron microscopy (TEM) elemen...Sodium-doped carbon nitride nanotubes (Nax-CNNTs) were prepared by a green and simple two-step method and applied in photocatalytic water splitting for the first time. Transmission electron microscopy (TEM) element mapping and X-ray photoelectron spectroscopy (XPS) measurements confirm that sodium was successfully introduced in the carbon nitride nanotubes (CNNTs), and the intrinsic structure of graphitic carbon nitride (g-C3N4) was also maintained in the products. Moreover, the porous structure of the CNNTs leads to relatively large specific surface areas. Photocatalytic tests indicate that the porous tubular structure and Na+ doping can synergistically enhance the hydrogen evolution rate under visible light (λ 〉 420 nm) irradiation in the presence of sacrificial agents, leading to a hydrogen evolution rate as high as 143 μmol·h-1 (20 mg catalyst). Moreover, other alkali metal-doped CNNTs, such as Lix-CNNTs and Kx-CNNTs, were tested; both materials were found to enhance the hydrogen evolution rate, but to a lower extent compared with the Nax-CNNTs. This highlights the general applicability of the present method to prepare alkali metal-doped CNNTs; a preliminary mechanism for the photocatalytic hydrogen evolution reaction in the Nax-CNNTs is also proposed.展开更多
The electronic structure of the heterojunction is the foundation of the study on its working mechanism. Models of the heterojunctions formed by an (8, 0) boron nitride nanotube and an (8, 0) carbon nanotube with C...The electronic structure of the heterojunction is the foundation of the study on its working mechanism. Models of the heterojunctions formed by an (8, 0) boron nitride nanotube and an (8, 0) carbon nanotube with C-B or C-N interface have been established. The structures of the above heterojunctions were optimized with first-principle calculations based on density functional theory. The rearrangements of the heterojunctions concentrate mainly on their interfaces. The highest occupied molecular orbital and the lowest unoccupied molecular orbital of the heterojunctions distribute in the carbon nanotube section. As the band offsets of the above heterojunctions are achieved with the average bond energy method, the band structure is plotted.展开更多
基金financially supported by the National Natural Science Foundation of China (21872065, 21763013, and 21503100)the Natural Science Foundation of Jiangxi Province (20192ACBL21027 and 20192BAB203007)the Project of Education Department of Jiangxi Province (GJJ170227)。
文摘Designing defect-engineered semiconductor heterojunctions can effectively promote the charge carrier separation.Herein,novel ceria(CeO2) quantum dots(QDs) decorated sulfur-doped carbon nitride nanotubes(SCN NTs) were synthesized via a thermal polycondensation coupled in situ depositionprecipitation method without use of template or surfactant.The structure and morphology studies indicate that ultrafine CeO2 QDs are well distributed inside and outside of SCN NTs offering highly dispersed active sites and a large contact interface between two components.This leads to the promoted formation of rich Ce^(3+) ion and oxygen vacancies as confirmed by XPS.The photocatalytic performance can be facilely modulated by the content of CeO2 QDs introduced in SCN matrix while bare CeO2 does not show activity of hydrogen production.The optimal catalyst with 10% of CeO2 loading yields a hydrogen evolution rate of 2923.8 μmol h-1 g-1 under visible light,remarkably higher than that of bare SCN and their physical mixtures.Further studies reveal that the abundant surface defects and the created 0 D/1 D junctions play a critical role in improving the separation and transfer of charge carriers,leading to superior solar hydrogen production and good stability.
基金The authors would like to thank the financial support from Sakura Science Program (Japan Science and Technology Agency), National Natural Science Foundation of China (Nos. 51627803, 51402348, 11474333, 91433205, 51421002, and 51372270) and the Knowledge Innovation Program of the Chinese Academy of Sciences.
文摘Sodium-doped carbon nitride nanotubes (Nax-CNNTs) were prepared by a green and simple two-step method and applied in photocatalytic water splitting for the first time. Transmission electron microscopy (TEM) element mapping and X-ray photoelectron spectroscopy (XPS) measurements confirm that sodium was successfully introduced in the carbon nitride nanotubes (CNNTs), and the intrinsic structure of graphitic carbon nitride (g-C3N4) was also maintained in the products. Moreover, the porous structure of the CNNTs leads to relatively large specific surface areas. Photocatalytic tests indicate that the porous tubular structure and Na+ doping can synergistically enhance the hydrogen evolution rate under visible light (λ 〉 420 nm) irradiation in the presence of sacrificial agents, leading to a hydrogen evolution rate as high as 143 μmol·h-1 (20 mg catalyst). Moreover, other alkali metal-doped CNNTs, such as Lix-CNNTs and Kx-CNNTs, were tested; both materials were found to enhance the hydrogen evolution rate, but to a lower extent compared with the Nax-CNNTs. This highlights the general applicability of the present method to prepare alkali metal-doped CNNTs; a preliminary mechanism for the photocatalytic hydrogen evolution reaction in the Nax-CNNTs is also proposed.
基金supported by the Pre-Research Foundation from the National Ministries and Commissions(No.51308040203).
文摘The electronic structure of the heterojunction is the foundation of the study on its working mechanism. Models of the heterojunctions formed by an (8, 0) boron nitride nanotube and an (8, 0) carbon nanotube with C-B or C-N interface have been established. The structures of the above heterojunctions were optimized with first-principle calculations based on density functional theory. The rearrangements of the heterojunctions concentrate mainly on their interfaces. The highest occupied molecular orbital and the lowest unoccupied molecular orbital of the heterojunctions distribute in the carbon nanotube section. As the band offsets of the above heterojunctions are achieved with the average bond energy method, the band structure is plotted.