Recently, the g-C3N4-based heterojunctions have been widely investigated for their greatly enhanced photogenerated carrier separation efficiency. However, most studies are based on the study of g-C3N4 powders. In this...Recently, the g-C3N4-based heterojunctions have been widely investigated for their greatly enhanced photogenerated carrier separation efficiency. However, most studies are based on the study of g-C3N4 powders. In this study, a novel TiN/C3N4/CdS nanotube arrays core/shell structure is designed to improve the photoelectrochemical catalytic performance of the g-C3N4-based heterojunctions. Among them, TiN nanotube arrays do not respond to simulated solar light, and thus only serve as an excellently conductive nanotube arrays backbone for supporting g-C3N4/CdS heterojunctions. g-C3N4 prepared by simple liquid atomic layer deposition, which possesses appropriate energy band position, mainly acts as the electron acceptor to transport and separate electrons. Deposited CdS quantum dots obtained by successive ionic layer adsorption reaction can effectively absorb visible light and thus act as a light absorber. The TiN/C3N4/CdS nanotube arrays core/shell structure could be verified by X-ray diffractions, Raman spectra, scanning electron microscopy, transmission electron microscopy, energy dispersive spectroscopy elemental mappings and X-ray photoelectron spectroscopy. Compared with TiN/C3N4 nanotube arrays, the TiN/C3N4/CdS samples greatly improve the photoelectrochemical performance, which can be evaluated by photoelectrochemical tests and photoelectrochemical catalytic degradation. Especially, the optimized photocurrent density of TiN/C3N4/CdS has almost 120 times improvement on TiN/C3N4 at 0 V bias under simulated sunlight, which can be ascribed to the effective expansion of the light absorption range and separation of electron-hole pairs.展开更多
Understanding of metal oxidation is very critical to corrosion control,catalysis synthesis,and advanced materials engineering.Metal oxidation is a very complex phenomenon,with many different processes which are couple...Understanding of metal oxidation is very critical to corrosion control,catalysis synthesis,and advanced materials engineering.Metal oxidation is a very complex phenomenon,with many different processes which are coupled and involved from the onset of reaction.In this work,the initial stage of oxidation on titanium surface was investigated in atomic scale by molecular dynamics(MD)simulations using a reactive force field(ReaxFF).We show that oxygen transport is the dominant process during the initial oxidation.Our simulation also demonstrate that a compressive stress was generated in the oxide layer which blocked the oxygen transport perpendicular to the Titanium(0001)surface and further prevented oxidation in the deeper layers.The mechanism of initial oxidation observed in this work can be also applicable to other self-limiting oxidation.展开更多
Adsorptive separation of acetylene(C_(2)H_(2))from carbon dioxide(CO_(2))is of great significance in petrochemical industry,but still remains as a daunting challenge by reason of their very similar molecular sizes/sha...Adsorptive separation of acetylene(C_(2)H_(2))from carbon dioxide(CO_(2))is of great significance in petrochemical industry,but still remains as a daunting challenge by reason of their very similar molecular sizes/shapes and physical properties.Herein,we reported a new perchlorate-based hybrid ultramicroporous material ZJU-194 that features the unique flexible-robust network decorated with rich bare oxygen atoms.By integrating the refined pore space as well as specific binding sites,the activated ZJU-194(ZJU-194a)enables a selective two-step gate-opening adsorption toward C_(2)H_(2),but blocks off the further uptake of CO_(2).It thus exhibits a very high C_(2)H_(2)/CO_(2)selectivity(22.4)at ambient conditions,which is superior to most reported MOF materials.Its complete separation for 50/50 C_(2)H_(2)/CO_(2)mixtures is further evidenced by the dynamic breakthrough experiments.展开更多
An atomic layer deposition (ALD) method has been employed to synthesize Fe3O4/graphene and Ni/graphene composites. The structure and microwave absorbing properties of the as-prepared composites are investigated. The...An atomic layer deposition (ALD) method has been employed to synthesize Fe3O4/graphene and Ni/graphene composites. The structure and microwave absorbing properties of the as-prepared composites are investigated. The surfaces of graphene are densely covered by Fe3O4 or Ni nanoparticles with a narrow size distribution, and the magnetic nanoparticles are well distributed on each graphene sheet without significant conglomeration or large vacancies. The coated graphene materials exhibit remarkably improved electromagnetic (EM) absorption properties compared to the pristine graphene. The optimal reflection loss (RL) reaches -46.4 dB at 15.6 GHz with a thickness of only 1.4 mm for the Fe3O4/graphene composites obtained by applying 100 cycles of Fe2O3 deposition followed by a hydrogen reduction. The enhanced absorption ability arises from the effective impedance matching, multiple interfacial polarization and increased magnetic loss from the added magnetic constituents. Moreover, compared with other recently reported materials, the composites have a lower filling ratio and smaller coating thickness resulting in significantly increased EM absorption properties. This demonstrates that nanoscale surface modification of magnetic particles on graphene by ALD is a very promising way to design lightweight and high-efficiency microwave absorbers.展开更多
Two perylene bisimides based non-fullerene small molecules, H-DIPBI and B-DIPBI, are applied into inverted planar heterojunction perovskite solar cells. The power conversion efficiency up to 11.6% has been achieved fo...Two perylene bisimides based non-fullerene small molecules, H-DIPBI and B-DIPBI, are applied into inverted planar heterojunction perovskite solar cells. The power conversion efficiency up to 11.6% has been achieved for device with B-DIPBI,indicating that non-fullerene acceptor can function as the electron transport layer to replace PCBM in perovskite solar cells.展开更多
Controlling the charge transfer and thus enhancing the excitons’lifetime are the key to the realization of efficient photoelectrochemical(PEC)devices.Moreover,fabrication of flexible and collapsible sensors can great...Controlling the charge transfer and thus enhancing the excitons’lifetime are the key to the realization of efficient photoelectrochemical(PEC)devices.Moreover,fabrication of flexible and collapsible sensors can greatly facilitate the implementation of smart PEC sensing devices into practical applications.Herein,we sagely designed and successfully fabricated three-dimensional flexible Au nanoparticles-decorated TiO_(2) nanotube arrays(Au@TiO2)for the efficient PEC biosensing of glucose.The Schottky barrier derived from the Au@TiO2 heterostructure efficiently separates the charge carriers at the junction interfaces,thus greatly increasing the concentration and lifetime of holes left in the valence band of TiO2.The separated holes further evidently generate the active hydroxyl radicals,which can specifically recognize and oxidize glucose.As a result,Au@TiO_(2) exhibits excellent photoelectric activity and selectivity,far superior to TiO_(2) without decorated Au nanoparticles.In addition,such asymmetric Au@TiO_(2) system has been proved to feature the intrinsic flexibility nature,since its PEC biosensing performance is almost unaffected under indirect light irradiation and serious tensile strain.展开更多
文摘Recently, the g-C3N4-based heterojunctions have been widely investigated for their greatly enhanced photogenerated carrier separation efficiency. However, most studies are based on the study of g-C3N4 powders. In this study, a novel TiN/C3N4/CdS nanotube arrays core/shell structure is designed to improve the photoelectrochemical catalytic performance of the g-C3N4-based heterojunctions. Among them, TiN nanotube arrays do not respond to simulated solar light, and thus only serve as an excellently conductive nanotube arrays backbone for supporting g-C3N4/CdS heterojunctions. g-C3N4 prepared by simple liquid atomic layer deposition, which possesses appropriate energy band position, mainly acts as the electron acceptor to transport and separate electrons. Deposited CdS quantum dots obtained by successive ionic layer adsorption reaction can effectively absorb visible light and thus act as a light absorber. The TiN/C3N4/CdS nanotube arrays core/shell structure could be verified by X-ray diffractions, Raman spectra, scanning electron microscopy, transmission electron microscopy, energy dispersive spectroscopy elemental mappings and X-ray photoelectron spectroscopy. Compared with TiN/C3N4 nanotube arrays, the TiN/C3N4/CdS samples greatly improve the photoelectrochemical performance, which can be evaluated by photoelectrochemical tests and photoelectrochemical catalytic degradation. Especially, the optimized photocurrent density of TiN/C3N4/CdS has almost 120 times improvement on TiN/C3N4 at 0 V bias under simulated sunlight, which can be ascribed to the effective expansion of the light absorption range and separation of electron-hole pairs.
基金Support of this work from the National Natural Science Foundation of China(Grant No.51361009)Work at Ames Laboratory was supported by the US Department of Energy,Basic Energy Sciences,Division of Materials Science and Engineering under Contract No.DE-AC02-07CH11358,including a grant of computer time at the National Energy Research Scientific Computing Centre(NERSC)in Berkeley,CA.
文摘Understanding of metal oxidation is very critical to corrosion control,catalysis synthesis,and advanced materials engineering.Metal oxidation is a very complex phenomenon,with many different processes which are coupled and involved from the onset of reaction.In this work,the initial stage of oxidation on titanium surface was investigated in atomic scale by molecular dynamics(MD)simulations using a reactive force field(ReaxFF).We show that oxygen transport is the dominant process during the initial oxidation.Our simulation also demonstrate that a compressive stress was generated in the oxide layer which blocked the oxygen transport perpendicular to the Titanium(0001)surface and further prevented oxidation in the deeper layers.The mechanism of initial oxidation observed in this work can be also applicable to other self-limiting oxidation.
基金supported by the National Natural Science Foundation of China(No.52003069)the Hainan Provincial Natural Science Foundation of China(No.520QN220).
文摘Adsorptive separation of acetylene(C_(2)H_(2))from carbon dioxide(CO_(2))is of great significance in petrochemical industry,but still remains as a daunting challenge by reason of their very similar molecular sizes/shapes and physical properties.Herein,we reported a new perchlorate-based hybrid ultramicroporous material ZJU-194 that features the unique flexible-robust network decorated with rich bare oxygen atoms.By integrating the refined pore space as well as specific binding sites,the activated ZJU-194(ZJU-194a)enables a selective two-step gate-opening adsorption toward C_(2)H_(2),but blocks off the further uptake of CO_(2).It thus exhibits a very high C_(2)H_(2)/CO_(2)selectivity(22.4)at ambient conditions,which is superior to most reported MOF materials.Its complete separation for 50/50 C_(2)H_(2)/CO_(2)mixtures is further evidenced by the dynamic breakthrough experiments.
文摘An atomic layer deposition (ALD) method has been employed to synthesize Fe3O4/graphene and Ni/graphene composites. The structure and microwave absorbing properties of the as-prepared composites are investigated. The surfaces of graphene are densely covered by Fe3O4 or Ni nanoparticles with a narrow size distribution, and the magnetic nanoparticles are well distributed on each graphene sheet without significant conglomeration or large vacancies. The coated graphene materials exhibit remarkably improved electromagnetic (EM) absorption properties compared to the pristine graphene. The optimal reflection loss (RL) reaches -46.4 dB at 15.6 GHz with a thickness of only 1.4 mm for the Fe3O4/graphene composites obtained by applying 100 cycles of Fe2O3 deposition followed by a hydrogen reduction. The enhanced absorption ability arises from the effective impedance matching, multiple interfacial polarization and increased magnetic loss from the added magnetic constituents. Moreover, compared with other recently reported materials, the composites have a lower filling ratio and smaller coating thickness resulting in significantly increased EM absorption properties. This demonstrates that nanoscale surface modification of magnetic particles on graphene by ALD is a very promising way to design lightweight and high-efficiency microwave absorbers.
基金supported by the National Natural Science Foundation of China(NSFC)(51473009)the International Science&Technology Cooperation Program of China(2014DFA52820)
文摘Two perylene bisimides based non-fullerene small molecules, H-DIPBI and B-DIPBI, are applied into inverted planar heterojunction perovskite solar cells. The power conversion efficiency up to 11.6% has been achieved for device with B-DIPBI,indicating that non-fullerene acceptor can function as the electron transport layer to replace PCBM in perovskite solar cells.
基金financially supported by the National Natural Science Foundation of China(Nos.61764003 and 51462008)the Major Science and Technology Planning Project of Hainan Province(No.ZDKJ201810)。
文摘Controlling the charge transfer and thus enhancing the excitons’lifetime are the key to the realization of efficient photoelectrochemical(PEC)devices.Moreover,fabrication of flexible and collapsible sensors can greatly facilitate the implementation of smart PEC sensing devices into practical applications.Herein,we sagely designed and successfully fabricated three-dimensional flexible Au nanoparticles-decorated TiO_(2) nanotube arrays(Au@TiO2)for the efficient PEC biosensing of glucose.The Schottky barrier derived from the Au@TiO2 heterostructure efficiently separates the charge carriers at the junction interfaces,thus greatly increasing the concentration and lifetime of holes left in the valence band of TiO2.The separated holes further evidently generate the active hydroxyl radicals,which can specifically recognize and oxidize glucose.As a result,Au@TiO_(2) exhibits excellent photoelectric activity and selectivity,far superior to TiO_(2) without decorated Au nanoparticles.In addition,such asymmetric Au@TiO_(2) system has been proved to feature the intrinsic flexibility nature,since its PEC biosensing performance is almost unaffected under indirect light irradiation and serious tensile strain.