In this work,a comparative study of three frequently employed modification techniques to g-C_(3)N_(4)(CN)nanosheets for the photocatalytic degradation of metribuzin(MET)under visible-light irradiation has been carried...In this work,a comparative study of three frequently employed modification techniques to g-C_(3)N_(4)(CN)nanosheets for the photocatalytic degradation of metribuzin(MET)under visible-light irradiation has been carried out in detail.The modification methods were coupling TiO_(2)nanoparticles(TO)as electron acceptors,nano-sized Fe_(2)O_(3)(FO)to construct a Z-scheme nanocomposite,and phosphate(HP)modification to promote O_(2)adsorption.The steady-state and transient-state surface photovoltage spectra and transient photoluminescence(PL)spectra confirmed that all the three modification techniques enhanced the charge separation with prolonged lifetimes and presented degradation activities in the order of TO/CN[FO/CN[HP/CN.The TO/CN nanocomposite showed the highest photocatalytic activity for MET degradation,with a sixfold higher rate than bulk CN.Liquid chromatography–tandem mass spectrometry and radical trapping experiments indicated that the increased activity was related to the synergetic effect of two radicals(·O^(2-) and ·OH)involved in the photocatalytic degradation pathway,which was different from the·OH radical-dominated pathway of bulk CN.This work reveals the importance of charge separation and the influence of the radical pathway and provides guidance for the design of high-efficiency photocatalysts.展开更多
A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles(NPs)were produced through single-step pyrolysis of FeCl_3–Ti(OBu)_4 laden agar biomass under NH_3 environment...A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles(NPs)were produced through single-step pyrolysis of FeCl_3–Ti(OBu)_4 laden agar biomass under NH_3 environment.The physiochemical properties of composites were characterized thoroughly.It has found that heating temperature and N-doping through NH_3-ambiance pyrolysis significantly influence the visible-light sensitivity and bandgap energy of composites.The catalytic activities of composites were measured by degradation of Methylene Blue(MB)in the presence or absence of H_2O_2 and visible-light irradiation.Our best catalyst(N–TiO_2–Fe_3O_4-biochar)exhibits rapid and high MB removal competency(99.99%)via synergism of adsorption,photodegradation,and Fenton-like reaction.Continuous production of O_2U^-and UOH radicles performs MB degradation and mineralization,confirmed by scavenging experiments and degradation product analysis.The local trap state Ti^(3+),Fe_3O_4,and N-carbon of the catalyst acted as active sites.It has suggested that the Ti^(3+)and N-doped dense carbon layer improve charge separation and shuttle that prolonged photo-Fenton like reaction.Moreover,the catalyst is highly stable,collectible,and recyclable up to 5 cycles with high MB degradation efficiency.This work provides a new insight into the synthesis of highly visible-light sensitized biocharsupported photocatalyst through NH_3-ambiance pyrolysis of NPs-laden biomass.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(Nos.21971057 and U1805255)the Natural Science Foundation of Heilongjiang Province(Nos.YQ2019B006 and LH2020B012)+2 种基金the Postdoctoral Research Foundation of Heilongjiang Province(No.LBH-Q19052)the Outstanding Youth Fund of Heilongjiang University(No.JCL201901)the Basic Scientific Research Expenses of Colleges and Universities in Heilongjiang Province(No.2020-KYYWF-1008).
文摘In this work,a comparative study of three frequently employed modification techniques to g-C_(3)N_(4)(CN)nanosheets for the photocatalytic degradation of metribuzin(MET)under visible-light irradiation has been carried out in detail.The modification methods were coupling TiO_(2)nanoparticles(TO)as electron acceptors,nano-sized Fe_(2)O_(3)(FO)to construct a Z-scheme nanocomposite,and phosphate(HP)modification to promote O_(2)adsorption.The steady-state and transient-state surface photovoltage spectra and transient photoluminescence(PL)spectra confirmed that all the three modification techniques enhanced the charge separation with prolonged lifetimes and presented degradation activities in the order of TO/CN[FO/CN[HP/CN.The TO/CN nanocomposite showed the highest photocatalytic activity for MET degradation,with a sixfold higher rate than bulk CN.Liquid chromatography–tandem mass spectrometry and radical trapping experiments indicated that the increased activity was related to the synergetic effect of two radicals(·O^(2-) and ·OH)involved in the photocatalytic degradation pathway,which was different from the·OH radical-dominated pathway of bulk CN.This work reveals the importance of charge separation and the influence of the radical pathway and provides guidance for the design of high-efficiency photocatalysts.
基金supported by the National Basic Research Program of China (973 Program, 2014CB238903)the National Natural Science Foundation of China (Nos. 41672144, 41173032, and 41373110)
文摘A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles(NPs)were produced through single-step pyrolysis of FeCl_3–Ti(OBu)_4 laden agar biomass under NH_3 environment.The physiochemical properties of composites were characterized thoroughly.It has found that heating temperature and N-doping through NH_3-ambiance pyrolysis significantly influence the visible-light sensitivity and bandgap energy of composites.The catalytic activities of composites were measured by degradation of Methylene Blue(MB)in the presence or absence of H_2O_2 and visible-light irradiation.Our best catalyst(N–TiO_2–Fe_3O_4-biochar)exhibits rapid and high MB removal competency(99.99%)via synergism of adsorption,photodegradation,and Fenton-like reaction.Continuous production of O_2U^-and UOH radicles performs MB degradation and mineralization,confirmed by scavenging experiments and degradation product analysis.The local trap state Ti^(3+),Fe_3O_4,and N-carbon of the catalyst acted as active sites.It has suggested that the Ti^(3+)and N-doped dense carbon layer improve charge separation and shuttle that prolonged photo-Fenton like reaction.Moreover,the catalyst is highly stable,collectible,and recyclable up to 5 cycles with high MB degradation efficiency.This work provides a new insight into the synthesis of highly visible-light sensitized biocharsupported photocatalyst through NH_3-ambiance pyrolysis of NPs-laden biomass.
