Pure bismuth（Bi） metal-modified graphitic carbon nitride（g-C3N4） composites（Bi-CN） with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the ox...Pure bismuth（Bi） metal-modified graphitic carbon nitride（g-C3N4） composites（Bi-CN） with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the oxidation of nitric oxide（NO） under visible-light irradiation.The inclusion of pure Bi metal in the g-C3N4 layers markedly improved the light absorption of the Bi-CN composites from the ultraviolet to the near-infrared region because of the typical surface plasmon resonance of Bi metal.The separation and transfer of photogenerated charge carriers were greatly accelerated by the presence of built-in Mott-Schottky effects at the interface between Bi metal and g-C3N4.As a result,the Bi-CN composite photocatalysts exhibited considerably enhanced efficiency in the photocatalytic removal of NO compared with that of Bi metal or g-C3N4 alone.The pomegranate-like structure of the Bi-CN composites and an explanation for their improved photocatalytic activity were proposed.This work not only provides a design for highly efficient g-C3N4-based photocatalysts through modification with Bi metal,but also offers new insights into the mechanistic understanding of g-C3N4-based photo catalysis.展开更多
Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode ...Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode is manufactured by depositing plasmonic nanoparticles of the non-noble metal Al on the surface of a TiO2/Cu2O core/shell heterojunction for the first time.The Al nanoparticles,which exhibit a surface plasmon resonance(SPR)effect and are substantially less expensive than noble metals such as Au and Ag,generate hot electron-hole pairs and amplify the electromagnetic field at the interface under illumination.The as-prepared TiO2/Cu2O/Al/Al2O3 photoelectrodes have an extended absorption range and enhanced carrier separation and transfer.Their photocurrent density of 4.52 mA·cm^-2 at 1.23 V vs.RHE represents an 1.84-fold improvement over that of TiO2/Cu2O.Specifically,the ultrathin Al2O3 passivation layer spontaneously generated on the surface of Al in air could act as a protective layer to significantly increase its stability.In this work,the synergistic effect of the heterojunctions and the SPR effect of the non-noble metal Al significantly improve the photoelectrode performance,providing a novel concept for the design of electrodes with good properties and high practicability.展开更多
Electrochemical （EC） reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique...Electrochemical （EC） reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique for chemical analysis, yet its application to EC reactions is hindered by the strong attenuation of infrared （IR） light in both electrodes and electrolytes. Here we demonstrate that by incorporating appropriate sub-wavelength plasmonic structures at the metal electrode, the IR field at the EC interface can be greatly enhanced via the excitation of surface plasmon. This scheme facilitates in situ vibrational spectroscopic studies, especially using the surface-specific sum-frequency generation technique.展开更多
The enhanced laser cooling performance of rare-earth-ions-doped glasses containing small particles is predicted. This is achieved by the enhancement of local field around rare earth ions, owing to the surface plasmon ...The enhanced laser cooling performance of rare-earth-ions-doped glasses containing small particles is predicted. This is achieved by the enhancement of local field around rare earth ions, owing to the surface plasmon resonance of small metallic particles. The role of energy transfer between ions and the particle is theoretical discussed. Depending on the particle size and the ion emission quantum efficiency, the enhancement of the absorption and the fluorescence is predicted. Moreover, taking Yb^3＋-doped ZBLAN as example, the cooling power and heat-light converting efficiency are calculated. It is finally concluded that the absorption and the fluorescence are greatly enhanced in these composite materials, the cooling power is increased compared to the bulk material.展开更多
In this study, we developed a highly sensitive dual-mode imaging system using gold nanoparticles （GNPs） conjugated to various fluorophores in solid phantoms. The system consists of fluorescence-lifetime imaging micr...In this study, we developed a highly sensitive dual-mode imaging system using gold nanoparticles （GNPs） conjugated to various fluorophores in solid phantoms. The system consists of fluorescence-lifetime imaging microscopy （FLIM） for surface imaging, diffusion reflection （DR） for deep-tissue imaging （up to 1 cm）, and metal-enhanced fluorescence （MEF）. We detected quenching in the fluorescent intensity （FI） for the conjugation of both gold nanospheres （GNS） and gold nanorods （GNRs） to Fluorescein, which has an excitation peak at a wavelength shorter than the surface plasmon resonance （SPR） of both types of GNPs. Enhanced FI was detected in conjugation to Rhodamine B （RhB） and Sulforhodamine B （SRB）, both with excitation peaks in the SPR regions of the GNPs. The enhanced FI was detected both in solution and in solid phantoms by the FLIM measurements. DR measurements detected the presence of GNRs within the solid phantoms by recording the dropped rates of light scattering in wavelengths corresponding to the absorption spectra of the GNRs. With the inclusion of MEF, this promising dual-mode imaging technique enables efficient and sensitive molecular and functional imaging.展开更多
Plasmonic bismuth(Bi^0)nanoparticle-decorated flower-like CeO2-δ(Bi^0/CeO2-δ)photocatalysts with abundant oxygen vacancies(OVs)were synthesized via a solvothermal method.The OVs can not only improve the separation o...Plasmonic bismuth(Bi^0)nanoparticle-decorated flower-like CeO2-δ(Bi^0/CeO2-δ)photocatalysts with abundant oxygen vacancies(OVs)were synthesized via a solvothermal method.The OVs can not only improve the separation of electron-hole pairs,but also facilitate the adsorption and activation of gas molecules(NO/O2).In addition,the Bi^0 nanoparticles can enhance the visible light response and prevent the recombination of charge carriers by virtue of the surface plasmon resonance(SPR)effect,achieving an excellent ability for NO elimination and NO2 inhibition under visible light irradiation.Density functional theory(DFT)calculations confirm that the Schottky barrier between Bi^0 and CeO2-δaccompanied with the OVs are pivotal for the migration of photogenerated charge carriers to involve in the photocatalytic NO removal.Trapping experiments and in situ FTIR spectroscopy were conducted to explore the mechanism of the photocatalytic NO removal,suggesting that the photocatalytic NO removal can be significantly enhanced by introducing abundant OVs and the involvement of Bi^0 metal nanoparticles.展开更多
Tip-enhanced Raman spectrum(TERS) is a scanning probe technique for acquiring chemical information at high spatial resolution and with high chemical sensitivity. The sensitivity of TERS with atomic force microscopy(AF...Tip-enhanced Raman spectrum(TERS) is a scanning probe technique for acquiring chemical information at high spatial resolution and with high chemical sensitivity. The sensitivity of TERS with atomic force microscopy(AFM) system is mainly determined by the metalized tips. Here, we report a fabrication protocol for AFM-TERS tips that incorporate a copper(Cu) primer film between a gold(Au) layer and a Si AFM tip. They were fabricated by coating the Si tip with a 2 nm Cu layer prior to adding a 20 nm Au layer. For top illumination TERS experiments, these tips exhibited superior TERS performance relative to that observed for tips coated with Au only. Samples included graphene, thiophenol and brilliant cresyl blue. The results may derive from the surface roughness of the tip apex and a Cu/Au synergism of local surface plasmon resonances.展开更多
We successfully investigate an optical bistability phenomenon in a layered structure consisting of Kretschmann configuration involving the Kerr-type nonlinear and the silver film. Pure theoretical approaches are emplo...We successfully investigate an optical bistability phenomenon in a layered structure consisting of Kretschmann configuration involving the Kerr-type nonlinear and the silver film. Pure theoretical approaches are employed to investigate that the surface plasmon could easily be coupled and both the reflection and transmission curves versus the incident intensity forms optical bistability. The transmission curves are greatly influenced by the thickness of the second silver film. These results may be useful for designing novel surface plasmon-based optical devices and will be essential for future classical and quantum information processes.展开更多
基金supported by the National Program on Key Basic Research Project (2016YFA0203000)the Early Career Scheme (ECS 809813) from the Research Grant Council, Hong Kong SAR Government+2 种基金the Croucher Foundation Visitorship for PRC Scholars 2015/16 at The Education University of Hong Kongthe National Natural Science Foundation of China (51672312, 21373275)the Program for New Century Excellent Talents in University (NCET-12-0668)~~
文摘Pure bismuth（Bi） metal-modified graphitic carbon nitride（g-C3N4） composites（Bi-CN） with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the oxidation of nitric oxide（NO） under visible-light irradiation.The inclusion of pure Bi metal in the g-C3N4 layers markedly improved the light absorption of the Bi-CN composites from the ultraviolet to the near-infrared region because of the typical surface plasmon resonance of Bi metal.The separation and transfer of photogenerated charge carriers were greatly accelerated by the presence of built-in Mott-Schottky effects at the interface between Bi metal and g-C3N4.As a result,the Bi-CN composite photocatalysts exhibited considerably enhanced efficiency in the photocatalytic removal of NO compared with that of Bi metal or g-C3N4 alone.The pomegranate-like structure of the Bi-CN composites and an explanation for their improved photocatalytic activity were proposed.This work not only provides a design for highly efficient g-C3N4-based photocatalysts through modification with Bi metal,but also offers new insights into the mechanistic understanding of g-C3N4-based photo catalysis.
文摘Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode is manufactured by depositing plasmonic nanoparticles of the non-noble metal Al on the surface of a TiO2/Cu2O core/shell heterojunction for the first time.The Al nanoparticles,which exhibit a surface plasmon resonance(SPR)effect and are substantially less expensive than noble metals such as Au and Ag,generate hot electron-hole pairs and amplify the electromagnetic field at the interface under illumination.The as-prepared TiO2/Cu2O/Al/Al2O3 photoelectrodes have an extended absorption range and enhanced carrier separation and transfer.Their photocurrent density of 4.52 mA·cm^-2 at 1.23 V vs.RHE represents an 1.84-fold improvement over that of TiO2/Cu2O.Specifically,the ultrathin Al2O3 passivation layer spontaneously generated on the surface of Al in air could act as a protective layer to significantly increase its stability.In this work,the synergistic effect of the heterojunctions and the SPR effect of the non-noble metal Al significantly improve the photoelectrode performance,providing a novel concept for the design of electrodes with good properties and high practicability.
文摘Electrochemical （EC） reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique for chemical analysis, yet its application to EC reactions is hindered by the strong attenuation of infrared （IR） light in both electrodes and electrolytes. Here we demonstrate that by incorporating appropriate sub-wavelength plasmonic structures at the metal electrode, the IR field at the EC interface can be greatly enhanced via the excitation of surface plasmon. This scheme facilitates in situ vibrational spectroscopic studies, especially using the surface-specific sum-frequency generation technique.
基金supported by the National Natural Science Foundation of China under Grant Nos.10434060 and 10674047the Doctor Foundation of the Ministry of Education under Grant No.20040269010Shanghai Priority Academic Discipline,and the 211 Foundation of the Ministry of Education Doctor Program Scholarship Fund of ECNU 2007
文摘The enhanced laser cooling performance of rare-earth-ions-doped glasses containing small particles is predicted. This is achieved by the enhancement of local field around rare earth ions, owing to the surface plasmon resonance of small metallic particles. The role of energy transfer between ions and the particle is theoretical discussed. Depending on the particle size and the ion emission quantum efficiency, the enhancement of the absorption and the fluorescence is predicted. Moreover, taking Yb^3＋-doped ZBLAN as example, the cooling power and heat-light converting efficiency are calculated. It is finally concluded that the absorption and the fluorescence are greatly enhanced in these composite materials, the cooling power is increased compared to the bulk material.
文摘In this study, we developed a highly sensitive dual-mode imaging system using gold nanoparticles （GNPs） conjugated to various fluorophores in solid phantoms. The system consists of fluorescence-lifetime imaging microscopy （FLIM） for surface imaging, diffusion reflection （DR） for deep-tissue imaging （up to 1 cm）, and metal-enhanced fluorescence （MEF）. We detected quenching in the fluorescent intensity （FI） for the conjugation of both gold nanospheres （GNS） and gold nanorods （GNRs） to Fluorescein, which has an excitation peak at a wavelength shorter than the surface plasmon resonance （SPR） of both types of GNPs. Enhanced FI was detected in conjugation to Rhodamine B （RhB） and Sulforhodamine B （SRB）, both with excitation peaks in the SPR regions of the GNPs. The enhanced FI was detected both in solution and in solid phantoms by the FLIM measurements. DR measurements detected the presence of GNRs within the solid phantoms by recording the dropped rates of light scattering in wavelengths corresponding to the absorption spectra of the GNRs. With the inclusion of MEF, this promising dual-mode imaging technique enables efficient and sensitive molecular and functional imaging.
基金supported by the National Natural Science Foundation of China(51772183,21673118 and 21972067)the Key Research and Development Program of Shaanxi Province(2018ZDCXL-SF-02-04)+1 种基金the Natural Science Foundation of Hubei Province(2019CFB225)the Fundamental Research Funds for the Central Universities(GK201903023 and GK201801005)。
文摘Plasmonic bismuth(Bi^0)nanoparticle-decorated flower-like CeO2-δ(Bi^0/CeO2-δ)photocatalysts with abundant oxygen vacancies(OVs)were synthesized via a solvothermal method.The OVs can not only improve the separation of electron-hole pairs,but also facilitate the adsorption and activation of gas molecules(NO/O2).In addition,the Bi^0 nanoparticles can enhance the visible light response and prevent the recombination of charge carriers by virtue of the surface plasmon resonance(SPR)effect,achieving an excellent ability for NO elimination and NO2 inhibition under visible light irradiation.Density functional theory(DFT)calculations confirm that the Schottky barrier between Bi^0 and CeO2-δaccompanied with the OVs are pivotal for the migration of photogenerated charge carriers to involve in the photocatalytic NO removal.Trapping experiments and in situ FTIR spectroscopy were conducted to explore the mechanism of the photocatalytic NO removal,suggesting that the photocatalytic NO removal can be significantly enhanced by introducing abundant OVs and the involvement of Bi^0 metal nanoparticles.
基金supported by the National Basic Research Program of China(2011YQ03012415,2011CB808700)the National Natural Science Foundation of China(21127901,233010,21121063)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB12020100)
文摘Tip-enhanced Raman spectrum(TERS) is a scanning probe technique for acquiring chemical information at high spatial resolution and with high chemical sensitivity. The sensitivity of TERS with atomic force microscopy(AFM) system is mainly determined by the metalized tips. Here, we report a fabrication protocol for AFM-TERS tips that incorporate a copper(Cu) primer film between a gold(Au) layer and a Si AFM tip. They were fabricated by coating the Si tip with a 2 nm Cu layer prior to adding a 20 nm Au layer. For top illumination TERS experiments, these tips exhibited superior TERS performance relative to that observed for tips coated with Au only. Samples included graphene, thiophenol and brilliant cresyl blue. The results may derive from the surface roughness of the tip apex and a Cu/Au synergism of local surface plasmon resonances.
基金supported by the National Basic Research Program of China (Grant No. 2010CB923202)
文摘We successfully investigate an optical bistability phenomenon in a layered structure consisting of Kretschmann configuration involving the Kerr-type nonlinear and the silver film. Pure theoretical approaches are employed to investigate that the surface plasmon could easily be coupled and both the reflection and transmission curves versus the incident intensity forms optical bistability. The transmission curves are greatly influenced by the thickness of the second silver film. These results may be useful for designing novel surface plasmon-based optical devices and will be essential for future classical and quantum information processes.
