Here,Ag2S nanoparticles on reduced graphene oxide（Ag2S NPs/RGO） nanocomposites with relatively good distribution are synthesized for the first time by conversing Ag NPs/RGO to Ag2S NPs/RGO via a facile hydrothermal ...Here,Ag2S nanoparticles on reduced graphene oxide（Ag2S NPs/RGO） nanocomposites with relatively good distribution are synthesized for the first time by conversing Ag NPs/RGO to Ag2S NPs/RGO via a facile hydrothermal sulfurization method.As an noval catalyst for the reduction of 4-nitrophenol（4-NP）,it only takes 5 min for Ag2S NPs/RGO to reduce 98% of 4-NP,and the rate constant of the composites is almost 13 times higher than that of Ag NPs/RGO composites.The high catalytic activity of Ag2S NPs/RGO can be attributed to the following three reasons：（1） Like metal complex catalysts,the Ag2S NPs is also rich with metal center Ag（δ^＋）,with pendant base S（δ） close to it,and thus the Ag and basic S function as the electron-acceptor and proton-acceptor centers,respectively,which facilitates the catalyst reaction;（2）RGO features the high adsorption ability toward 4-NP which provides a high concentration of 4-NP near the Ag2S NPs;and（3） electron transfer from RGO to Ag2S NPs,facilitating the uptake of electrons by 4-NP molecules.展开更多
CdIn2S4 microspheres were synthesized by a facile hydrothermal method with the temperature ranging from 120 to 200 ℃. X-ray diffraction, UV-vis diffuse reflectance spectroscopy, nitrogen sorption analysis, X-ray phot...CdIn2S4 microspheres were synthesized by a facile hydrothermal method with the temperature ranging from 120 to 200 ℃. X-ray diffraction, UV-vis diffuse reflectance spectroscopy, nitrogen sorption analysis, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy were used to characterize the products. It was found that the crystallographic structure and optical property of the products synthesized at different temperature were almost the same. The SBEX of CdIn2S4 products decreased when the synthesized temperature increased, and the largest SBET was 33.16 m2 g-1 （120 ℃ sample）. The degradation of methyl orange （MO） under the visible-light irradiation had been used as a probe reaction to investigate the photocatalytic activity of the as-prepared CdIn2S4, which showed that the CdIn2S4 sample synthesized at 120 ℃ presented the best photocatalytic activity for MO degradation.展开更多
Hierarchical heterostructure photocatalysts with broad spectrum solar light utilization,particularly in the nearinfrared(NIR)region,are emerging classes of advanced photocatalytic materials for solar-driven CO2 conver...Hierarchical heterostructure photocatalysts with broad spectrum solar light utilization,particularly in the nearinfrared(NIR)region,are emerging classes of advanced photocatalytic materials for solar-driven CO2 conversion into value-added chemical feedstocks.Herein,a novel two-demensional/three-demensional(2 D/3 D)hierarchical composite is hydrothermally synthesized by assembling vertically-aligned ZnIn2 S4(ZIS)nanowall arrays on nitrogen-doped graphene foams(NGF).The prepared ZIS/NGF composite shows enhancement in photothermal conversion ability and selective CO2 capture as well as solar-driven CO2 photoreduction.At273 K and 1 atm,the ZIS/NGF composite with 1.0 wt%NGF achieves a comparably high CO2-to-N2 selectivity of 30.1,with an isosteric heat of CO2 adsorption of 48.2 kJ mol^-1.And in the absence of cocatalysts and sacrificial agents,the ZIS/NGF composite with cyclability converts CO2 into CH4,CO and CH3 OH under simulated solar light illumination,with the respective evolution rates about 9.1,3.5,and 5.9 times higher than that of the pristine ZIS.In-depth analysis using in-situ irradiated X-ray photoelectron spectroscopy(ISI-XPS)in conjunction with Kelvin probe measurements reveals the underlying charge transfer pathway and process from ZIS to NGF.展开更多
Nanomaterial shapes can have profound effects on material properties, and therefore offer an efficient way to improve the performances of designed materials and devices. The rational fabrication of multidimensional ar...Nanomaterial shapes can have profound effects on material properties, and therefore offer an efficient way to improve the performances of designed materials and devices. The rational fabrication of multidimensional architectures such as one dimensional （1D）-two dimensional （2D） hybrid nanomaterials can integrate the merits of individual components and provide enhanced functionality. However, it is still very challenging to fabricate 1D/2D architectures because of the different growth mechanisms of the nanostructures. Here, we present a new solvent- mediated, surface reaction-driven growth route for synthesis of CdS nanowire （NW）/CdIn2S4 nanosheet （NS） 1D/2D architectures. The as-obtained CdS NW/ CdIn2S4 NS structures exhibit much higher visible-light-responsive photocatalytic activities for water splitting than the individual components. The CdS NW/CdIn2S4 NS heterostructure was further fabricated into photoelectrodes, which achieved a considerable photocurrent density of 2.85 mA·cm^-2 at 0 V vs. the reversible hydrogen electrode （RHE） without use of any co-catalysts. This represents one of the best results from a CdS-based photoelectrochemical （PEC） cell. Both the multidimensional nature and type II band alignment of the 1D/2D CdS/CdIn2S4 heterostructure contribute to the enhanced photocatalyfic and photoelectrochemical activity. The present work not only provides a new strategy for designing multidimensional 1D/2D heterostructures, but also documents the development of highly efficient energy conversion catalysts.展开更多
文摘Here,Ag2S nanoparticles on reduced graphene oxide（Ag2S NPs/RGO） nanocomposites with relatively good distribution are synthesized for the first time by conversing Ag NPs/RGO to Ag2S NPs/RGO via a facile hydrothermal sulfurization method.As an noval catalyst for the reduction of 4-nitrophenol（4-NP）,it only takes 5 min for Ag2S NPs/RGO to reduce 98% of 4-NP,and the rate constant of the composites is almost 13 times higher than that of Ag NPs/RGO composites.The high catalytic activity of Ag2S NPs/RGO can be attributed to the following three reasons：（1） Like metal complex catalysts,the Ag2S NPs is also rich with metal center Ag（δ^＋）,with pendant base S（δ） close to it,and thus the Ag and basic S function as the electron-acceptor and proton-acceptor centers,respectively,which facilitates the catalyst reaction;（2）RGO features the high adsorption ability toward 4-NP which provides a high concentration of 4-NP near the Ag2S NPs;and（3） electron transfer from RGO to Ag2S NPs,facilitating the uptake of electrons by 4-NP molecules.
基金Natural Science Foundation of China(11804003)Natural Science Foundation of Anhui Province(1908085QF277)+1 种基金Open Foundation of Nano-mineral Materials and Application of the Ministry of Education Engineering Research Center(NGM2019KF029)The University-Industry Collaboration Program with Anhui Dushi High-tech Glass Co.Ltd.(880111)~~
基金financially supported by the Natural Science Foundation of Fujian Province (2011J05024)
文摘CdIn2S4 microspheres were synthesized by a facile hydrothermal method with the temperature ranging from 120 to 200 ℃. X-ray diffraction, UV-vis diffuse reflectance spectroscopy, nitrogen sorption analysis, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy were used to characterize the products. It was found that the crystallographic structure and optical property of the products synthesized at different temperature were almost the same. The SBEX of CdIn2S4 products decreased when the synthesized temperature increased, and the largest SBET was 33.16 m2 g-1 （120 ℃ sample）. The degradation of methyl orange （MO） under the visible-light irradiation had been used as a probe reaction to investigate the photocatalytic activity of the as-prepared CdIn2S4, which showed that the CdIn2S4 sample synthesized at 120 ℃ presented the best photocatalytic activity for MO degradation.
基金supported by the National Natural Science Foundation of China (51961135303, 51932007, 21871217 and U1705251)the National Key Research and Development Program of China (2018YFB1502001)Innovative Research Funds of SKLWUT (2017-ZD-4)
文摘Hierarchical heterostructure photocatalysts with broad spectrum solar light utilization,particularly in the nearinfrared(NIR)region,are emerging classes of advanced photocatalytic materials for solar-driven CO2 conversion into value-added chemical feedstocks.Herein,a novel two-demensional/three-demensional(2 D/3 D)hierarchical composite is hydrothermally synthesized by assembling vertically-aligned ZnIn2 S4(ZIS)nanowall arrays on nitrogen-doped graphene foams(NGF).The prepared ZIS/NGF composite shows enhancement in photothermal conversion ability and selective CO2 capture as well as solar-driven CO2 photoreduction.At273 K and 1 atm,the ZIS/NGF composite with 1.0 wt%NGF achieves a comparably high CO2-to-N2 selectivity of 30.1,with an isosteric heat of CO2 adsorption of 48.2 kJ mol^-1.And in the absence of cocatalysts and sacrificial agents,the ZIS/NGF composite with cyclability converts CO2 into CH4,CO and CH3 OH under simulated solar light illumination,with the respective evolution rates about 9.1,3.5,and 5.9 times higher than that of the pristine ZIS.In-depth analysis using in-situ irradiated X-ray photoelectron spectroscopy(ISI-XPS)in conjunction with Kelvin probe measurements reveals the underlying charge transfer pathway and process from ZIS to NGF.
基金This work was financially supported by the National Natural Science Foundation of China （Nos. 51372173, 21673160, and 51420105002）, Natural Science Foundation of Zhejiang for Distinguished Young Scholars （No. LR16B010002）, Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure （No. SKL201409SIC）, and startup funds of Syracuse University.
文摘Nanomaterial shapes can have profound effects on material properties, and therefore offer an efficient way to improve the performances of designed materials and devices. The rational fabrication of multidimensional architectures such as one dimensional （1D）-two dimensional （2D） hybrid nanomaterials can integrate the merits of individual components and provide enhanced functionality. However, it is still very challenging to fabricate 1D/2D architectures because of the different growth mechanisms of the nanostructures. Here, we present a new solvent- mediated, surface reaction-driven growth route for synthesis of CdS nanowire （NW）/CdIn2S4 nanosheet （NS） 1D/2D architectures. The as-obtained CdS NW/ CdIn2S4 NS structures exhibit much higher visible-light-responsive photocatalytic activities for water splitting than the individual components. The CdS NW/CdIn2S4 NS heterostructure was further fabricated into photoelectrodes, which achieved a considerable photocurrent density of 2.85 mA·cm^-2 at 0 V vs. the reversible hydrogen electrode （RHE） without use of any co-catalysts. This represents one of the best results from a CdS-based photoelectrochemical （PEC） cell. Both the multidimensional nature and type II band alignment of the 1D/2D CdS/CdIn2S4 heterostructure contribute to the enhanced photocatalyfic and photoelectrochemical activity. The present work not only provides a new strategy for designing multidimensional 1D/2D heterostructures, but also documents the development of highly efficient energy conversion catalysts.
