A series of Au/g-C3N4(Au/CN)nanocomposites were successfully prepared,where g-C3N4 nanosheets(CN NSs)served as a substrate for the growth of different sized Au nanoparticles(Au NPs)using the constant temperature bath-...A series of Au/g-C3N4(Au/CN)nanocomposites were successfully prepared,where g-C3N4 nanosheets(CN NSs)served as a substrate for the growth of different sized Au nanoparticles(Au NPs)using the constant temperature bath-reduction method.The effect of Au NP size on electron transfer efficiency between the interfaces of the nanocomposite was studied.The three-dimensional finite-difference time-domain results revealed that larger Au NPs showed increased strength of the localized surface plasmon resonance effect.An increased number of high-energy electrons were available for transfer from Au NPs to CN under the visible light irradiation,inhibiting electron transfer from CN to Au NPs.Photoelectrochemical performance analysis showed that smaller Au NPs exhibited higher separation efficiency of the electron-hole pairs photo-generated with reasonable distribution density.These results are favorable for the improvement of photocatalytic performance.Compared to other nanocomposites,the 3-Au/CN sample(prepared using 3 mL HAuCl4 solution)with reasonable distribution density and small Au NPs exhibited the best photodegradation activity(92.66%)of RhB in 30 min under the visible light irradiation and photoreduction performance of CO2 to CO and CH4 with yields of 77.5 and 38.5μmol/g,respectively,in 8 h under UV light irradiation.Considering the experimental results in the context of the literature,a corresponding size-dependent photocatalytic mechanism was proposed.展开更多
The active site amount of photocatalysts,being the key factors in photocatalytic reactions,directly affects the photocatalytic performance of the photocatalyst.Pristine graphitic carbon nitride(g‐C_(3)N_(4))exhibits ...The active site amount of photocatalysts,being the key factors in photocatalytic reactions,directly affects the photocatalytic performance of the photocatalyst.Pristine graphitic carbon nitride(g‐C_(3)N_(4))exhibits moderate photocatalytic activity due to insufficient active sites.In this study,cyano‐modified porous g‐C_(3)N_(4)nanosheets(MCN‐0.5)were synthesized through molecular self‐assembly and alkali‐assisted strategies.The cyano group acted as the active site of the photocatalytic reaction,because the good electron‐withdrawing property of the cyano group promoted carrier separation.Benefiting from the effect of the active sites,MCN‐0.5 exhibited significantly enhanced photocatalytic activity for CO2 reduction under visible light irradiation.Notably,the photocatalytic activity of MCN‐0.5 was significantly reduced when the cyano groups were removed by hydrochloric acid(HCl)treatment,further verifying the role of cyano groups as active sites.The photoreduction of Pt nanoparticles provided an intuitive indication that the introduction of cyano groups provided more active sites for the photocatalytic reaction.Furthermore,the controlled experiments showed that g‐C_(3)N_(4)grafted with cyano groups using melamine as the precursor exhibited enhanced photocatalytic activity,which proved the versatility of the strategy for enhancing the activity of g‐C_(3)N_(4)via cyano group modification.In situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations were used to investigate the mechanism of enhanced photocatalytic activity for CO2 reduction by cyano‐modified g‐C_(3)N_(4).This work provides a promising route for promoting efficient solar energy conversion by designing active sites in photocatalysts.展开更多
Converting solar energy into hydrogen and hydrocarbon fuels through photocatalytic H2production and CO2photoreduction is a highly promising approach to address growing demand for clean andrenewable energy resources.Ho...Converting solar energy into hydrogen and hydrocarbon fuels through photocatalytic H2production and CO2photoreduction is a highly promising approach to address growing demand for clean andrenewable energy resources.However,solar‐to‐fuel conversion efficiencies of current photocatalysts are not sufficient to meet commercial requirements.The narrow window of solar energy that can be used has been identified as a key reason behind such low photocatalytic reaction efficiencies.The use of photonic crystals,formed from multiple material components,has been demonstrated to be an effective way of improving light harvesting.Within these nanostructures,the slow‐photon effect,a manifestation of light‐propagation control,considerably enhances the interaction between light and the semiconductor components.This article reviews recent developments in the applications of photonic crystals to photocatalytic H2production and CO2reduction based on slow photons.These advances show great promise for improving light harvesting in solar‐energy conversion technologies.展开更多
基金supported by the National Natural Science Foundation of China(21776117 and 21576125)China Postdoctoral Science Foundation(2017M611716 and 2017M611734)+1 种基金Six Talent Peaks Project in Jiangsu Province(XCL-014)Zhenjiang Science and Technology Program(SH2016012)~~
文摘A series of Au/g-C3N4(Au/CN)nanocomposites were successfully prepared,where g-C3N4 nanosheets(CN NSs)served as a substrate for the growth of different sized Au nanoparticles(Au NPs)using the constant temperature bath-reduction method.The effect of Au NP size on electron transfer efficiency between the interfaces of the nanocomposite was studied.The three-dimensional finite-difference time-domain results revealed that larger Au NPs showed increased strength of the localized surface plasmon resonance effect.An increased number of high-energy electrons were available for transfer from Au NPs to CN under the visible light irradiation,inhibiting electron transfer from CN to Au NPs.Photoelectrochemical performance analysis showed that smaller Au NPs exhibited higher separation efficiency of the electron-hole pairs photo-generated with reasonable distribution density.These results are favorable for the improvement of photocatalytic performance.Compared to other nanocomposites,the 3-Au/CN sample(prepared using 3 mL HAuCl4 solution)with reasonable distribution density and small Au NPs exhibited the best photodegradation activity(92.66%)of RhB in 30 min under the visible light irradiation and photoreduction performance of CO2 to CO and CH4 with yields of 77.5 and 38.5μmol/g,respectively,in 8 h under UV light irradiation.Considering the experimental results in the context of the literature,a corresponding size-dependent photocatalytic mechanism was proposed.
文摘The active site amount of photocatalysts,being the key factors in photocatalytic reactions,directly affects the photocatalytic performance of the photocatalyst.Pristine graphitic carbon nitride(g‐C_(3)N_(4))exhibits moderate photocatalytic activity due to insufficient active sites.In this study,cyano‐modified porous g‐C_(3)N_(4)nanosheets(MCN‐0.5)were synthesized through molecular self‐assembly and alkali‐assisted strategies.The cyano group acted as the active site of the photocatalytic reaction,because the good electron‐withdrawing property of the cyano group promoted carrier separation.Benefiting from the effect of the active sites,MCN‐0.5 exhibited significantly enhanced photocatalytic activity for CO2 reduction under visible light irradiation.Notably,the photocatalytic activity of MCN‐0.5 was significantly reduced when the cyano groups were removed by hydrochloric acid(HCl)treatment,further verifying the role of cyano groups as active sites.The photoreduction of Pt nanoparticles provided an intuitive indication that the introduction of cyano groups provided more active sites for the photocatalytic reaction.Furthermore,the controlled experiments showed that g‐C_(3)N_(4)grafted with cyano groups using melamine as the precursor exhibited enhanced photocatalytic activity,which proved the versatility of the strategy for enhancing the activity of g‐C_(3)N_(4)via cyano group modification.In situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations were used to investigate the mechanism of enhanced photocatalytic activity for CO2 reduction by cyano‐modified g‐C_(3)N_(4).This work provides a promising route for promoting efficient solar energy conversion by designing active sites in photocatalysts.
文摘Converting solar energy into hydrogen and hydrocarbon fuels through photocatalytic H2production and CO2photoreduction is a highly promising approach to address growing demand for clean andrenewable energy resources.However,solar‐to‐fuel conversion efficiencies of current photocatalysts are not sufficient to meet commercial requirements.The narrow window of solar energy that can be used has been identified as a key reason behind such low photocatalytic reaction efficiencies.The use of photonic crystals,formed from multiple material components,has been demonstrated to be an effective way of improving light harvesting.Within these nanostructures,the slow‐photon effect,a manifestation of light‐propagation control,considerably enhances the interaction between light and the semiconductor components.This article reviews recent developments in the applications of photonic crystals to photocatalytic H2production and CO2reduction based on slow photons.These advances show great promise for improving light harvesting in solar‐energy conversion technologies.
