A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride(g-C3N4)nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework(MOF)is proposed in th...A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride(g-C3N4)nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework(MOF)is proposed in this study.Specifically,Co-MOF as an electron donor is capable of transferring the photogenerated electrons in the lowest unoccupied molecular orbital(LUMO)to the conduction band of g-C3N4 to facilitate charge separation.As expected,the prepared Co-MOF/g-C3N4 nanocomposites display excellent visible-light-driven photocatalytic CO2 reduction activities.The CO production rate of 6.75μmol g–1 h–1 and CH4 evolution rate of 5.47μmol g–1 h–1 are obtained,which are approximately 2 times those obtained with the original g-C3N4 under the same conditions.Based on a series of analyses,it is shown that the introduction of Co-MOF not only broadens the range of visible-light absorption but also enhances the charge separation,which improves the photocatalytic activity of g-C3N4 to a higher level.In particular,the hydroxyl radical(·OH)experiment was operated under 590 nm(single-wavelength)irradiation,which further proved that the photogenerated electrons in the LUMO of Co-MOF can successfully migrate to g-C3N4.This work may provide an important strategy for the design of highly efficient g-C3N4-based photocatalysts for CO2 reduction.展开更多
Constructing binary heterojunctions is an important strategy to improve the photocatalytic performance of graphitic carbon nitride(g‐C3N4).In this paper,a novel g‐C3N4 nanosheet‐based composite was constructed via ...Constructing binary heterojunctions is an important strategy to improve the photocatalytic performance of graphitic carbon nitride(g‐C3N4).In this paper,a novel g‐C3N4 nanosheet‐based composite was constructed via in situ growth of bismuth oxyiodide(BiOI)nanoplates on the surface of g‐C3N4 nanosheets.The crystal phase,microstructure,optical absorption and textural properties of the synthesized photocatalysts were analyzed by X‐ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),ultraviolet‐visible(UV‐vis)diffuse reflectance spectroscopy(DRS),and nitrogen adsorption‐desorption isotherm measurements.The BiOI/g‐C3N4 nanosheet composite showed high activity and recyclability for the photodegradation of the target pollutant rhodamine B(RhB).The conversion of RhB(20 mg L?1)by the photocatalyst was nearly 100%after 50 min under visible‐light irradiation.The high photoactivity of the BiOI/g‐C3N4 nanosheet composite can be attributed to the enhanced visible‐light absorption of the g‐C3N4 nanosheets sensitized by BiOI nanoplates as well as the high charge separation efficiency obtained by the establishment of an internal electric field between the n‐type g‐C3N4 and p‐type BiOI.Based on the characterization and experimental results,a double‐transfer mechanism of the photoinduced electrons in the BiOI/g‐C3N4 nanosheet composite was proposed to explain its activity.This work represents a new strategy to understand and realize the design and synthesis of g‐C3N4 nanosheet‐based heterojunctions that display highly efficient charge separation and transfer.展开更多
PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution o...PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g^–1 h^–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g^–1 h^–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.展开更多
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
基金supported by the National Natural Science Foundation of China(21871079,21501052)the Outstanding Youth Project of Natural Science Foundation of Heilongjiang Province(YQ2019B006)~~
文摘A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride(g-C3N4)nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework(MOF)is proposed in this study.Specifically,Co-MOF as an electron donor is capable of transferring the photogenerated electrons in the lowest unoccupied molecular orbital(LUMO)to the conduction band of g-C3N4 to facilitate charge separation.As expected,the prepared Co-MOF/g-C3N4 nanocomposites display excellent visible-light-driven photocatalytic CO2 reduction activities.The CO production rate of 6.75μmol g–1 h–1 and CH4 evolution rate of 5.47μmol g–1 h–1 are obtained,which are approximately 2 times those obtained with the original g-C3N4 under the same conditions.Based on a series of analyses,it is shown that the introduction of Co-MOF not only broadens the range of visible-light absorption but also enhances the charge separation,which improves the photocatalytic activity of g-C3N4 to a higher level.In particular,the hydroxyl radical(·OH)experiment was operated under 590 nm(single-wavelength)irradiation,which further proved that the photogenerated electrons in the LUMO of Co-MOF can successfully migrate to g-C3N4.This work may provide an important strategy for the design of highly efficient g-C3N4-based photocatalysts for CO2 reduction.
文摘Constructing binary heterojunctions is an important strategy to improve the photocatalytic performance of graphitic carbon nitride(g‐C3N4).In this paper,a novel g‐C3N4 nanosheet‐based composite was constructed via in situ growth of bismuth oxyiodide(BiOI)nanoplates on the surface of g‐C3N4 nanosheets.The crystal phase,microstructure,optical absorption and textural properties of the synthesized photocatalysts were analyzed by X‐ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),ultraviolet‐visible(UV‐vis)diffuse reflectance spectroscopy(DRS),and nitrogen adsorption‐desorption isotherm measurements.The BiOI/g‐C3N4 nanosheet composite showed high activity and recyclability for the photodegradation of the target pollutant rhodamine B(RhB).The conversion of RhB(20 mg L?1)by the photocatalyst was nearly 100%after 50 min under visible‐light irradiation.The high photoactivity of the BiOI/g‐C3N4 nanosheet composite can be attributed to the enhanced visible‐light absorption of the g‐C3N4 nanosheets sensitized by BiOI nanoplates as well as the high charge separation efficiency obtained by the establishment of an internal electric field between the n‐type g‐C3N4 and p‐type BiOI.Based on the characterization and experimental results,a double‐transfer mechanism of the photoinduced electrons in the BiOI/g‐C3N4 nanosheet composite was proposed to explain its activity.This work represents a new strategy to understand and realize the design and synthesis of g‐C3N4 nanosheet‐based heterojunctions that display highly efficient charge separation and transfer.
基金supported by the National Natural Science Foundation of China(51572295,21273285,21003157)the Beijing Nova Program(2008B76)the Science Foundation of China University of Petroleum Beijing(KYJJ2012-06-20 and 2462016YXBS05)~~
文摘PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g^–1 h^–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g^–1 h^–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.
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.
