采用超声辅助室温原位沉淀法合成BC/Bi_(4)O_(5)Br_(2)光催化剂,在可见光下对比了TiO_(2)体系、BC/Bi_(4)O_(5)Br_(2)体系以及BC/Bi_(4)O_(5)Br_(2)耦合过一硫酸盐(PMS)体系处理渗滤液尾水的效果。考察了BC/Bi_(4)O_(5)Br_(2)耦合PMS体...采用超声辅助室温原位沉淀法合成BC/Bi_(4)O_(5)Br_(2)光催化剂,在可见光下对比了TiO_(2)体系、BC/Bi_(4)O_(5)Br_(2)体系以及BC/Bi_(4)O_(5)Br_(2)耦合过一硫酸盐(PMS)体系处理渗滤液尾水的效果。考察了BC/Bi_(4)O_(5)Br_(2)耦合PMS体系中PMS投加量和反应时间的影响,通过紫外可见光谱、三维荧光图谱分析渗滤液尾水有机物成分。结果表明:BC/Bi_(4)O_(5)Br_(2)耦合PMS体系对腐殖质的去除效果较另外两体系的效果优异,BC/Bi_(4)O_(5)Br_(2)对COD、腐殖质(A_(254))、色度(CN)的去除率分别为13.07%、12.74%、52.19%,BOD_(5)/COD从0.08提升至0.18。BC/Bi_(4)O_(5)Br_(2)耦合PMS体系中,0.1 g BC/Bi_(4)O_(5)Br_(2)耦合0.20 g PMS体系对渗滤液尾水有机物有良好的降解效果,尤其在反应开始的前0.5 h作用效果明显,1.5 h后降解效率不再明显增加。BC/Bi_(4)O_(5)Br_(2)耦合PMS体系对TOC的最大去除率为30.5%,较BC/Bi_(4)O_(5)Br_(2)体系提高16.5%;对腐殖质的最大去除率为53.97%,较BC/Bi_(4)O_(5)Br_(2)体系提升41.5%。紫外可见光谱、三维荧光图谱表明渗滤液尾水以类腐殖质为主。研究结果可为非均相耦合过一硫酸盐光催化处理渗滤液尾水提供一定参考。展开更多
Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions...Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.展开更多
The fabrication of heterojunction catalysts is an effective strategy to enhance charge separation efficiency,thus boosting the performance of photocatalysts.This work presents the synthesis and investigation of a nove...The fabrication of heterojunction catalysts is an effective strategy to enhance charge separation efficiency,thus boosting the performance of photocatalysts.This work presents the synthesis and investigation of a novel KNbO_(3)/Bi_(4)O_(5)Br_(2) heterostructure catalyst for photocatalytic N_(2)-to-NH_(3) conversion under light illumination.While morphology analysis revealed KNbO_(3) microcubes embedded within Bi_(4)O_(5)Br_(2) nanosheets,the composite exhibited no significant improvement in specific surface area or optical property compared to Bi_(4)O_(5)Br_(2) due to the relatively wide band gap and low surface area of KNbO_(3).The main contribution lies in the enhanced separation efficiency of photogenerated electrons and holes.Besides,the band structure analysis suggests that KNbO_(3) and Bi_(4)O_(5)Br_(2) exhibit suitable band potentials to form a type II heterojunction.Benefiting from the higher Fermi level of KNbO_(3) than Bi_(4)O_(5)Br_(2),the electron drift at the contact region thus occurs and leads to the formation of a built-in electric field with the direction from KNbO_(3) to Bi_(4)O_(5)Br_(2),accelerating electron migration and improving the operational efficiency of the photocatalysts.Consequently,the KNbO_(3)/Bi_(4)O_(5)Br_(2) catalyst shows an increased photoactivity,achieving an NH_(3) generation rate 1.78 and 1.58 times those of KNbO_(3) and Bi_(4)O_(5)Br_(2),respectively.This work may offer valuable insights for the design and synthesis of heterojunction composite photocatalysts.展开更多
Bi_(2)O_(2)CO_(3)(BOC)/Bi_(4)O_5Br_(2)(BOB)/reduced graphene oxide(rGO)Z-scheme heterojunction with promising photocatalytic properties was synthesized via a facile one-pot room-temperature method.Ultra-thin nanosheet...Bi_(2)O_(2)CO_(3)(BOC)/Bi_(4)O_5Br_(2)(BOB)/reduced graphene oxide(rGO)Z-scheme heterojunction with promising photocatalytic properties was synthesized via a facile one-pot room-temperature method.Ultra-thin nanosheets of BOC and BOB were grown in situ on r GO.The formed 2D/2D direct Z-scheme heterojunction of BOC/BOB with oxygen vacancies(OVs)effectively leads to lower negative electron reduction potential of BOB as well as higher positive hole oxidation potential of BOC,showing improved reduction/oxidation ability.Particularly,rGO is an acceptor of the electrons from the conduction band of BOC.Its dual roles significantly improve the transfer performance of photo-induced charge carriers and accelerate their separation.With layered nanosheet structure,rich OVs,high specific surface area,and increased utilization efficiency of visible light,the multiple synergistic effects of BOC/BOB/rGO can achieve effective generation and separation of the electron-holes,thereby generating more·O_(2)^(-)and h^(+).The photocatalytic reduction efficiency of CO_(2)to CO(12.91μmol/(g·hr))is three times higher than that of BOC(4.18μmol/(g·hr)).Moreover,it also achieved almost 100%removal of Rhodamine B and cyanobacterial cells within 2 hours.展开更多
One key strategy to enhance photocatalytic performance is to improve the transfer and separation efficiency of photogenerated carriers by building optimized heterojunctions.Herein,novel Bi_(4)O_5Br_(2)/NH_(2)-MIL-125(...One key strategy to enhance photocatalytic performance is to improve the transfer and separation efficiency of photogenerated carriers by building optimized heterojunctions.Herein,novel Bi_(4)O_5Br_(2)/NH_(2)-MIL-125(Ti)Z-scheme heterojunctions are fabricated and used as photocatalysts for organic pollutant photodegradation.The NH_(2)-MIL-125(Ti)nanosheets are exfoliated via a self-developed alkali solution stripping approach and then uniformly decorated on Bi_(4)O_(5)Br_(2).The as-prepared Bi_(4)O_(5)Br_(2)/NH_(2)-MIL-125(Ti)presents more than 90%degradation of various pollutants,outperforming the counterpart individual ones.The various characterization results suggest that the enhanced degradation rate is due to the more intimate face-to-face interfacial contact of the lamellar Z-scheme heterojunction materials,in which the migration path of carriers from the material's interior to the surface can be reduced,in turn enhancing migration efficiency and separation capability significantly.A possible photocatalytic reaction mechanism is proposed based on the photoelectric behaviors,radical trapping experiments and liquid chromatography mass spectrometry analysis.This work promotes the development of new photocatalytic materials for heterojunctions with face-to-face interfacial contacts,as well as the effective purification of wastewater in environmental remediation.展开更多
Herein,a series of three-dimensionally ordered macroporous(3DOM)Bi_(4)O_(5)Br_(2)photocatalysts with different macropore sizes were successfully fabricated via a polymethyl methacrylate(PMMA)template method.The photoc...Herein,a series of three-dimensionally ordered macroporous(3DOM)Bi_(4)O_(5)Br_(2)photocatalysts with different macropore sizes were successfully fabricated via a polymethyl methacrylate(PMMA)template method.The photocatalytic activity for phenol degradation over 3DOM Bi_(4)O_(5)Br_(2)first increased and then decreased with the rise in macropore size.Specifically,3DOM Bi_(4)O_(5)Br_(2)-255(macropore diameter ca.170 nm)exhibits the best photocatalytic activity in the static system,which is about 4.5,7.3,and 11.9 times higher than those of bulk Bi_(4)O_(5)Br_(2),Bi_(2)WO_(6),and g-C_(3)N_(4),respectively.Meanwhile,high phenol conversion(75%)is also obtained over 3DOM Bi_(4)O_(5)Br_(2)-255 in the flow system under full spectrum irradiation.Furthermore,3DOM Bi_(4)O_(5)Br_(2)-255 also shows strong mineralization capacity owing to the downward shift of valance band position(0.15 V)as compared with Bi_(4)O_(5)Br_(2).Total organic carbon(TOC)removal rate over 3DOM Bi_(4)O_(5)Br_(2)-255(62%)is much higher than that of Bi_(4)O_(5)Br_(2)(17%).The enhancement in photocatalytic performance of 3DOM Bi_(4)O_(5)Br_(2)-255 is attributable to its better phenol adsorption,O_(2)activation,and charge separation and transfer abilities.This work combines the advantages of 3D structure and surface dangling bonds,providing new possibilities for designing highly efficient photocatalysts for pollutants removal.展开更多
Photocatalytic process represents a promising approach to overcome the pollution challenge associated with the antibiotics-containing wastewater.This study provides a green,efficient and novel approach to remove cepha...Photocatalytic process represents a promising approach to overcome the pollution challenge associated with the antibiotics-containing wastewater.This study provides a green,efficient and novel approach to remove cephalosporins,particularly cefoperazone sodium(CFP).Bi_(4)O_(5)Br_(2) was chosen for the first time to systematically study its degradation for CFP,including the analysis of material structure,degradation performance,the structure and toxicity of the transformation products,etc.The degradation rate results indicated that Bi_(4)O_(5)Br_(2) had an excellent catalytic activity leading to 78%CFP removal compared with the pure BiOBr(38%)within 120 min of visible light irradiation.In addition,the Bi_(4)O_(5)Br_(2) presents high stability and good organic carbon removal efficiency.The effects of the solution p H(3.12-8.75)on catalytic activity revealed that CFP was mainly photocatalyzed under acidic conditions and hydrolyzed under alkaline conditions.Combined with active species and degradation product identification,the photocatalytic degradation pathways of CFP by Bi_(4)O_(5)Br_(2) was proposed,including hydrolysis,oxidation,reduction and decarboxylation.Most importantly,the identified products were all hydrolysis rather than oxidation byproducts transformed from the intermediate ofβ-lactam bond cleavage in CFP molecule,quite different from the mostly previous studies.Furthermore,the final products were demonstrated to be less toxic through the toxicity analysis.Overall,this study illustrates the detailed mechanism of CFP degradation by Bi_(4)O_(5)Br_(2) and confirms Bi_(4)O_(5)Br_(2) to be a promising material for the photodegradation of CFP.展开更多
Inorganic photocatalysts have been regarded as a promising candidate in the domain of tumor photodynamic therapy(PDT)due to their inspirational photocatalytic activity.In this study,a Bi_(4)O_(5)Br_(2)photocatalyst wa...Inorganic photocatalysts have been regarded as a promising candidate in the domain of tumor photodynamic therapy(PDT)due to their inspirational photocatalytic activity.In this study,a Bi_(4)O_(5)Br_(2)photocatalyst was synthesized and it exhibited effective photo-killing activity of A549 cells(a human lung carcinoma epithelial cell line)in vitro.On this basis,we modified Bi_(4)O_(5)Br_(2)with carbon quantum dots(CQDs)via a hydrolysis method at room temperature,which resulted in an improved photo-killing effect of Bi_(4)O_(5)Br_(2)to A549 cells.The samples and the interaction between samples and cells were fully characterized.It has been found that the loading of CQDs on Bi_(4)O_(5)Br_(2)can reduce the hydration ratio,increase the cellular uptake and improve the photogenerated reactive oxygen species(ROS)as compared with pristine Bi_(4)O_(5)Br_(2).Electron spin resonance(ESR)analysis and radical-trapping experiments manifested that the ROS contributed to PDT may be·O^(2-)and ·OH.This study may provide a useful strategy to ameliorate the penetrability,cell compatibility and PDT effect upon cancer cells of other inorganic photocatalysts.展开更多
文摘采用超声辅助室温原位沉淀法合成BC/Bi_(4)O_(5)Br_(2)光催化剂,在可见光下对比了TiO_(2)体系、BC/Bi_(4)O_(5)Br_(2)体系以及BC/Bi_(4)O_(5)Br_(2)耦合过一硫酸盐(PMS)体系处理渗滤液尾水的效果。考察了BC/Bi_(4)O_(5)Br_(2)耦合PMS体系中PMS投加量和反应时间的影响,通过紫外可见光谱、三维荧光图谱分析渗滤液尾水有机物成分。结果表明:BC/Bi_(4)O_(5)Br_(2)耦合PMS体系对腐殖质的去除效果较另外两体系的效果优异,BC/Bi_(4)O_(5)Br_(2)对COD、腐殖质(A_(254))、色度(CN)的去除率分别为13.07%、12.74%、52.19%,BOD_(5)/COD从0.08提升至0.18。BC/Bi_(4)O_(5)Br_(2)耦合PMS体系中,0.1 g BC/Bi_(4)O_(5)Br_(2)耦合0.20 g PMS体系对渗滤液尾水有机物有良好的降解效果,尤其在反应开始的前0.5 h作用效果明显,1.5 h后降解效率不再明显增加。BC/Bi_(4)O_(5)Br_(2)耦合PMS体系对TOC的最大去除率为30.5%,较BC/Bi_(4)O_(5)Br_(2)体系提高16.5%;对腐殖质的最大去除率为53.97%,较BC/Bi_(4)O_(5)Br_(2)体系提升41.5%。紫外可见光谱、三维荧光图谱表明渗滤液尾水以类腐殖质为主。研究结果可为非均相耦合过一硫酸盐光催化处理渗滤液尾水提供一定参考。
文摘Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.
基金supported by the National Natural Science Foundation of China (Grant No.22172144)the Key Research and Development Program of Zhejiang Province (Grant No.2023C03148).
文摘The fabrication of heterojunction catalysts is an effective strategy to enhance charge separation efficiency,thus boosting the performance of photocatalysts.This work presents the synthesis and investigation of a novel KNbO_(3)/Bi_(4)O_(5)Br_(2) heterostructure catalyst for photocatalytic N_(2)-to-NH_(3) conversion under light illumination.While morphology analysis revealed KNbO_(3) microcubes embedded within Bi_(4)O_(5)Br_(2) nanosheets,the composite exhibited no significant improvement in specific surface area or optical property compared to Bi_(4)O_(5)Br_(2) due to the relatively wide band gap and low surface area of KNbO_(3).The main contribution lies in the enhanced separation efficiency of photogenerated electrons and holes.Besides,the band structure analysis suggests that KNbO_(3) and Bi_(4)O_(5)Br_(2) exhibit suitable band potentials to form a type II heterojunction.Benefiting from the higher Fermi level of KNbO_(3) than Bi_(4)O_(5)Br_(2),the electron drift at the contact region thus occurs and leads to the formation of a built-in electric field with the direction from KNbO_(3) to Bi_(4)O_(5)Br_(2),accelerating electron migration and improving the operational efficiency of the photocatalysts.Consequently,the KNbO_(3)/Bi_(4)O_(5)Br_(2) catalyst shows an increased photoactivity,achieving an NH_(3) generation rate 1.78 and 1.58 times those of KNbO_(3) and Bi_(4)O_(5)Br_(2),respectively.This work may offer valuable insights for the design and synthesis of heterojunction composite photocatalysts.
基金supported by the National Natural Science Foundation of China(Nos.51602281 and 52100014)the Natural Science Foundation of Jiangsu Province(No.BK20180938)the Yangzhou University High-end Talent Support Program and the“Qinglan Project”of Jiangsu Universities。
文摘Bi_(2)O_(2)CO_(3)(BOC)/Bi_(4)O_5Br_(2)(BOB)/reduced graphene oxide(rGO)Z-scheme heterojunction with promising photocatalytic properties was synthesized via a facile one-pot room-temperature method.Ultra-thin nanosheets of BOC and BOB were grown in situ on r GO.The formed 2D/2D direct Z-scheme heterojunction of BOC/BOB with oxygen vacancies(OVs)effectively leads to lower negative electron reduction potential of BOB as well as higher positive hole oxidation potential of BOC,showing improved reduction/oxidation ability.Particularly,rGO is an acceptor of the electrons from the conduction band of BOC.Its dual roles significantly improve the transfer performance of photo-induced charge carriers and accelerate their separation.With layered nanosheet structure,rich OVs,high specific surface area,and increased utilization efficiency of visible light,the multiple synergistic effects of BOC/BOB/rGO can achieve effective generation and separation of the electron-holes,thereby generating more·O_(2)^(-)and h^(+).The photocatalytic reduction efficiency of CO_(2)to CO(12.91μmol/(g·hr))is three times higher than that of BOC(4.18μmol/(g·hr)).Moreover,it also achieved almost 100%removal of Rhodamine B and cyanobacterial cells within 2 hours.
基金financially supported by the National Natural Science Foundation of China(No.51302061)the Natural Science Foundation of Hebei province(Nos.E2014201076,E2020201021 and E2023201019)+3 种基金the Research Innovation Team of College of Chemistry and Environmental Science of Hebei University(No.hxkytd2102)Shenzhen Science and Technology Innovation Committee(No.JCYJ20200109141412308)Bintuan Science and Technology Program(Nos.2020DB002 and 2022DB009)CWO funding of Ghent University。
文摘One key strategy to enhance photocatalytic performance is to improve the transfer and separation efficiency of photogenerated carriers by building optimized heterojunctions.Herein,novel Bi_(4)O_5Br_(2)/NH_(2)-MIL-125(Ti)Z-scheme heterojunctions are fabricated and used as photocatalysts for organic pollutant photodegradation.The NH_(2)-MIL-125(Ti)nanosheets are exfoliated via a self-developed alkali solution stripping approach and then uniformly decorated on Bi_(4)O_(5)Br_(2).The as-prepared Bi_(4)O_(5)Br_(2)/NH_(2)-MIL-125(Ti)presents more than 90%degradation of various pollutants,outperforming the counterpart individual ones.The various characterization results suggest that the enhanced degradation rate is due to the more intimate face-to-face interfacial contact of the lamellar Z-scheme heterojunction materials,in which the migration path of carriers from the material's interior to the surface can be reduced,in turn enhancing migration efficiency and separation capability significantly.A possible photocatalytic reaction mechanism is proposed based on the photoelectric behaviors,radical trapping experiments and liquid chromatography mass spectrometry analysis.This work promotes the development of new photocatalytic materials for heterojunctions with face-to-face interfacial contacts,as well as the effective purification of wastewater in environmental remediation.
基金This work was supported by the National Natural Science Foundation of China(Nos.22206102,21872077,and 21621003)the National Key Research and Development Program of China(No.2020YFA0710304)the China Postdoctoral Science Foundation(No.2021M700078).
文摘Herein,a series of three-dimensionally ordered macroporous(3DOM)Bi_(4)O_(5)Br_(2)photocatalysts with different macropore sizes were successfully fabricated via a polymethyl methacrylate(PMMA)template method.The photocatalytic activity for phenol degradation over 3DOM Bi_(4)O_(5)Br_(2)first increased and then decreased with the rise in macropore size.Specifically,3DOM Bi_(4)O_(5)Br_(2)-255(macropore diameter ca.170 nm)exhibits the best photocatalytic activity in the static system,which is about 4.5,7.3,and 11.9 times higher than those of bulk Bi_(4)O_(5)Br_(2),Bi_(2)WO_(6),and g-C_(3)N_(4),respectively.Meanwhile,high phenol conversion(75%)is also obtained over 3DOM Bi_(4)O_(5)Br_(2)-255 in the flow system under full spectrum irradiation.Furthermore,3DOM Bi_(4)O_(5)Br_(2)-255 also shows strong mineralization capacity owing to the downward shift of valance band position(0.15 V)as compared with Bi_(4)O_(5)Br_(2).Total organic carbon(TOC)removal rate over 3DOM Bi_(4)O_(5)Br_(2)-255(62%)is much higher than that of Bi_(4)O_(5)Br_(2)(17%).The enhancement in photocatalytic performance of 3DOM Bi_(4)O_(5)Br_(2)-255 is attributable to its better phenol adsorption,O_(2)activation,and charge separation and transfer abilities.This work combines the advantages of 3D structure and surface dangling bonds,providing new possibilities for designing highly efficient photocatalysts for pollutants removal.
基金the National Natural Science Foundation of China(Nos.21972073,21677086 and 21577077)Hubei Province Introduces Foreign Talents and Intelligence Projects(No.2019BJH004)+2 种基金China Postdoctoral Science Foundation(No.2018M640721)Postdoctoral Science Foundation of Hubei Province(No.G83)Open Fund of Engineering Research Center of Eco-environment in Three Gorges Reservoir Region(No.KF2019-02)。
文摘Photocatalytic process represents a promising approach to overcome the pollution challenge associated with the antibiotics-containing wastewater.This study provides a green,efficient and novel approach to remove cephalosporins,particularly cefoperazone sodium(CFP).Bi_(4)O_(5)Br_(2) was chosen for the first time to systematically study its degradation for CFP,including the analysis of material structure,degradation performance,the structure and toxicity of the transformation products,etc.The degradation rate results indicated that Bi_(4)O_(5)Br_(2) had an excellent catalytic activity leading to 78%CFP removal compared with the pure BiOBr(38%)within 120 min of visible light irradiation.In addition,the Bi_(4)O_(5)Br_(2) presents high stability and good organic carbon removal efficiency.The effects of the solution p H(3.12-8.75)on catalytic activity revealed that CFP was mainly photocatalyzed under acidic conditions and hydrolyzed under alkaline conditions.Combined with active species and degradation product identification,the photocatalytic degradation pathways of CFP by Bi_(4)O_(5)Br_(2) was proposed,including hydrolysis,oxidation,reduction and decarboxylation.Most importantly,the identified products were all hydrolysis rather than oxidation byproducts transformed from the intermediate ofβ-lactam bond cleavage in CFP molecule,quite different from the mostly previous studies.Furthermore,the final products were demonstrated to be less toxic through the toxicity analysis.Overall,this study illustrates the detailed mechanism of CFP degradation by Bi_(4)O_(5)Br_(2) and confirms Bi_(4)O_(5)Br_(2) to be a promising material for the photodegradation of CFP.
基金This research was financially supported by the National Natural Science Foundation of China(Nos.21303116,21676178 and 21706179).
文摘Inorganic photocatalysts have been regarded as a promising candidate in the domain of tumor photodynamic therapy(PDT)due to their inspirational photocatalytic activity.In this study,a Bi_(4)O_(5)Br_(2)photocatalyst was synthesized and it exhibited effective photo-killing activity of A549 cells(a human lung carcinoma epithelial cell line)in vitro.On this basis,we modified Bi_(4)O_(5)Br_(2)with carbon quantum dots(CQDs)via a hydrolysis method at room temperature,which resulted in an improved photo-killing effect of Bi_(4)O_(5)Br_(2)to A549 cells.The samples and the interaction between samples and cells were fully characterized.It has been found that the loading of CQDs on Bi_(4)O_(5)Br_(2)can reduce the hydration ratio,increase the cellular uptake and improve the photogenerated reactive oxygen species(ROS)as compared with pristine Bi_(4)O_(5)Br_(2).Electron spin resonance(ESR)analysis and radical-trapping experiments manifested that the ROS contributed to PDT may be·O^(2-)and ·OH.This study may provide a useful strategy to ameliorate the penetrability,cell compatibility and PDT effect upon cancer cells of other inorganic photocatalysts.