Biomass chitosan(CS)was used as a template,graphitic phase carbon nitride(g-C_(3)N_(4))with high nitrogen content and certain catalytic activity was used as a dopant,and nano-transition metal cobalt(Co)was used as a c...Biomass chitosan(CS)was used as a template,graphitic phase carbon nitride(g-C_(3)N_(4))with high nitrogen content and certain catalytic activity was used as a dopant,and nano-transition metal cobalt(Co)was used as a catalytic center point.The carbon aerogel(C(CS)/g-C_(3)N_(4)/Co)with a three-dimensional network-like structure was prepared by assembling the three materials through experimental operations such as freeze-drying and high-temperature carbonization.It was demonstrated by scanning and transmission characterization that the CS in the carbon aerogel could provide more active sites for the cobalt nanoparticles,and the doping of graphite-phase carbon nitride as a template dispersed the cobalt nanoparticles and changed the conductivity of the CS.To investigate the catalytic effect of carbon aerogel on ammonium perchlorate(AP),it was investigated by differential thermal analyzer and TG thermal analysis.This carbon aerogel was very effective in catalyzing AP,and the 10 wt% content of the catalyst reduced the AP pyrolysis peak from 703.9 to 595.5 K.And to further investigate the synergistic effect of the three materials,further carbon aerogels such as C(CS)/Co,g-C_(3)N_(4)/Co were prepared and applied to catalyze AP,and the same ratio reduced the AP pyrolysis peak by 98.1℃ and 97.7℃.This result indicates a synergistic effect of the assembly of the three materials.展开更多
Visible-light-driven photocatalysis is a promising technology for the treatment of dye wastewater.In this work,a novel photocatalyst of K-doped g-C_(3)N_(4) loaded on magnetic attapulgite(ATP)(Kω-g-C_(3)N_(4)@ATP-Fe_...Visible-light-driven photocatalysis is a promising technology for the treatment of dye wastewater.In this work,a novel photocatalyst of K-doped g-C_(3)N_(4) loaded on magnetic attapulgite(ATP)(Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4))with excellent visible light photocatalytic properties and stability were successfully prepared and characterized.The removal efficiency of Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) for malachite green(MG)was studied,and the degradation mechanism was analyzed and proposed.It was found that the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst possessed excellent degradation efficiency of over 98.0%for the MG dye wastewater under optimal conditions.Moreover,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) materials possessed good recyclability with a removal rate over 82%after 4 cycles.Under visible light condition,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst produce radicals of·OH and O_(2)^(-)to degrade the MG dyes,which was supported by electron paramagnetic resonance(EPR)and radical trapping experiments.In addition,the LC-MS analysis interpreted the degradation pathways and intermediates of MG in the solution.The findings in this work indicate that the prepared photocatalytic material has excellent degradation efficiency for MG and can be applied in dye wastewater treatment.展开更多
Over the past decade, graphitic carbon nitride(g-C_(3)N_(4)) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C_(3)N_(4) is stil...Over the past decade, graphitic carbon nitride(g-C_(3)N_(4)) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C_(3)N_(4) is still confronted with a general fatal issue of insufficient supply of thermodynamically active photocarriers due to its inferior solar harvesting ability and sluggish charge transfer dynamics. Fortunately, this could be significantly alleviated by the “all-in-one” defect engineering strategy, which enables a simultaneous amelioration of both textural uniqueness and intrinsic electronic band structures. To this end, we have summarized an unprecedently comprehensive discussion on defect controls including the vacancy/non-metallic dopant creation with optimized electronic band structure and electronic density, metallic doping with ultraactive coordinated environment(M–N_(x), M–C_(2)N_(2), M–O bonding), functional group grafting with optimized band structure, and promoted crystallinity with extended conjugation π system with weakened interlayered van der Waals interaction. Among them, the defect states induced by various defect types such as N vacancy, P/S/halogen dopants, and cyano group in boosting solar harvesting and accelerating photocarrier transfer have also been emphasized. More importantly, the shallow defect traps identified by femtosecond transient absorption spectra(fs-TAS) have also been highlighted. It is believed that this review would pave the way for future readers with a unique insight into a more precise defective g-C_(3)N_(4) “customization”, motivating more profound thinking and flourishing research outputs on g-C_(3)N_(4)-based photocatalysis.展开更多
基金the financial support received from the Natural Science Foundation of China(21875192)Outstanding Youth Science and Technology Talents Program of Sichuan(no.19JCQN0085)Open Project of State Key Laboratory of Environment-friendly Energy Materials(Southwest University of Science and Technology,No.22fksy18)。
文摘Biomass chitosan(CS)was used as a template,graphitic phase carbon nitride(g-C_(3)N_(4))with high nitrogen content and certain catalytic activity was used as a dopant,and nano-transition metal cobalt(Co)was used as a catalytic center point.The carbon aerogel(C(CS)/g-C_(3)N_(4)/Co)with a three-dimensional network-like structure was prepared by assembling the three materials through experimental operations such as freeze-drying and high-temperature carbonization.It was demonstrated by scanning and transmission characterization that the CS in the carbon aerogel could provide more active sites for the cobalt nanoparticles,and the doping of graphite-phase carbon nitride as a template dispersed the cobalt nanoparticles and changed the conductivity of the CS.To investigate the catalytic effect of carbon aerogel on ammonium perchlorate(AP),it was investigated by differential thermal analyzer and TG thermal analysis.This carbon aerogel was very effective in catalyzing AP,and the 10 wt% content of the catalyst reduced the AP pyrolysis peak from 703.9 to 595.5 K.And to further investigate the synergistic effect of the three materials,further carbon aerogels such as C(CS)/Co,g-C_(3)N_(4)/Co were prepared and applied to catalyze AP,and the same ratio reduced the AP pyrolysis peak by 98.1℃ and 97.7℃.This result indicates a synergistic effect of the assembly of the three materials.
基金funded by the National Natural Science Foundation of China(22078138)the“Thousand Talents Plan”of Jiangxi Province(Jxsq2018101018)key projects of the Natural Science Foundation of Jiangxi Province(20202ACBL203009).
文摘Visible-light-driven photocatalysis is a promising technology for the treatment of dye wastewater.In this work,a novel photocatalyst of K-doped g-C_(3)N_(4) loaded on magnetic attapulgite(ATP)(Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4))with excellent visible light photocatalytic properties and stability were successfully prepared and characterized.The removal efficiency of Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) for malachite green(MG)was studied,and the degradation mechanism was analyzed and proposed.It was found that the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst possessed excellent degradation efficiency of over 98.0%for the MG dye wastewater under optimal conditions.Moreover,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) materials possessed good recyclability with a removal rate over 82%after 4 cycles.Under visible light condition,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst produce radicals of·OH and O_(2)^(-)to degrade the MG dyes,which was supported by electron paramagnetic resonance(EPR)and radical trapping experiments.In addition,the LC-MS analysis interpreted the degradation pathways and intermediates of MG in the solution.The findings in this work indicate that the prepared photocatalytic material has excellent degradation efficiency for MG and can be applied in dye wastewater treatment.
基金the support of the Australia Research Council (ARC) through the Discovery Project (DP230101040)the Natural Science Foundation of Shandong Province (ZR2022QB139, No. ZR2020KF025)+3 种基金the Starting Research Fund (Grant No. 20210122) from the Ludong Universitythe Natural Science Foundation of China (12274190) from the Ludong Universitythe support of the Shandong Youth Innovation Team Introduction and Education Programthe Special Fund for Taishan Scholars Project (No. tsqn202211186) in Shandong Province。
文摘Over the past decade, graphitic carbon nitride(g-C_(3)N_(4)) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C_(3)N_(4) is still confronted with a general fatal issue of insufficient supply of thermodynamically active photocarriers due to its inferior solar harvesting ability and sluggish charge transfer dynamics. Fortunately, this could be significantly alleviated by the “all-in-one” defect engineering strategy, which enables a simultaneous amelioration of both textural uniqueness and intrinsic electronic band structures. To this end, we have summarized an unprecedently comprehensive discussion on defect controls including the vacancy/non-metallic dopant creation with optimized electronic band structure and electronic density, metallic doping with ultraactive coordinated environment(M–N_(x), M–C_(2)N_(2), M–O bonding), functional group grafting with optimized band structure, and promoted crystallinity with extended conjugation π system with weakened interlayered van der Waals interaction. Among them, the defect states induced by various defect types such as N vacancy, P/S/halogen dopants, and cyano group in boosting solar harvesting and accelerating photocarrier transfer have also been emphasized. More importantly, the shallow defect traps identified by femtosecond transient absorption spectra(fs-TAS) have also been highlighted. It is believed that this review would pave the way for future readers with a unique insight into a more precise defective g-C_(3)N_(4) “customization”, motivating more profound thinking and flourishing research outputs on g-C_(3)N_(4)-based photocatalysis.
