This study presents the successful synthesis of a novel Z-scheme heterojunction composite film consisting of Ag/Bi_(2)MoO_(6)/BiOBr through electrochemical processes and ionexchange techniques,followed by the photodep...This study presents the successful synthesis of a novel Z-scheme heterojunction composite film consisting of Ag/Bi_(2)MoO_(6)/BiOBr through electrochemical processes and ionexchange techniques,followed by the photodeposition of noble metal silver(Ag)onto the composite structure.The catalytic efficiency of semiconductor photocatalysts is greatly improved by utilizing the localized surface plasmon resonance(LSPR)effect observed in Ag nanoparticles(NPs).Furthermore,the noble metal Ag serves as an intermediary bridge facilitating charge transfer between Bi_(2)MoO_(6)and BiOBr,while the formation of a Schottky barrier effectively inhibits the recombination of photo-generated electron-hole pairs.As a result,the Ag-deposited Bi_(2)MoO_(6)/BiOBr film exhibits superior photocatalytic performance in the reduction of CO_(2)compared to its unmodified counterpart.Our experimental results indicate a non-linear relationship between Ag deposition and the efficiency of photocatalytic CO_(2)reduction to CO,characterized by an initial increase in efficiency followed by a decline.The optimized 1.5%-Ag/Bi_(2)MoO_(6)/BiOBr film demonstrates exceptional photocatalytic activity,attaining a CO production rate of 13.65μmol/(g·h).This research explores the fundamental mechanisms that lead to improved photocatalytic CO_(2)reduction capabilities of the Ag/Bi_(2)MoO_(6)/BiOBr film.Our research offers important perspectives for the thoughtful design and production of highly efficient photocatalysts,which are essential for advancing sustainable energy solutions.展开更多
The excessive use of pesticides has exacerbated environmental pollution due to herbicide residues,while their persistent toxicity poses serious challenges to global ecological security.A magnetically recyclable CoFe_(...The excessive use of pesticides has exacerbated environmental pollution due to herbicide residues,while their persistent toxicity poses serious challenges to global ecological security.A magnetically recyclable CoFe_(2)O_(4)/BiOBr S-scheme heterojunctions was prepared by microwave-assisted co-precipitation method for photocatalytic degradation of Diuron(DUR) in water.The formation of S-scheme heterojunction enhances electron transfer and charge separation,which was demonstrated by free radical trapping,electrochemical experiments,and DFT calculations.The magnetic CoFe_(2)O_(4)/BiOBr catalysts can achieve 99.9 %removal of diuron in 50 min under visible light irradiation.Furthermore,the system maintains stable performance across a broad p H range(3-9),enabling adaptation to diverse water environments,effective elimination of multiple pollutants,and strong resistance to ionic interference.Using magnetic recovery,CoFe_(2)O_(4)/BiOBr exhibits a high removal rate of 99 % and a markedly low ion leaching rate(<20 μg/L) after six cycles photocatalytic process,confirming its excellent stability and durability.According to HPLCQTOF-MS and DFT calculation,the main ways of DUR degradation include dechlorinated hydroxylation,dealkylation and hydroxylation of aromatic ring and side chain.Toxicity analysis showed that the toxicity of the intermediates generated during degradation was generally lower than that of DUR.The magnetic CoFe_(2)O_(4)/BiOBr S-scheme heterojunction developed in this study exhibits excellent photocatalytic performance,high applicability,good stability,and durability,providing an effective magnetic for the removal of refractory pollutants.展开更多
CO_(2) photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse effect.Herein,the 5,10,15,20-tetra(4-carboxyphenyl)porphyrin cobalt(II)(CoTCPP)h...CO_(2) photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse effect.Herein,the 5,10,15,20-tetra(4-carboxyphenyl)porphyrin cobalt(II)(CoTCPP)has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr composite.The as-prepared CoTCPP/BiOBr-2 composite shows optimized photocatalytic performance for CO_(2) conversion into CO and CH_(4) upon irradiation with 300 W Xe lamp,which is 2.03 and 2.58 times compared to that of BiOBr,respectively.The introduced CoTCPP significantly enhanced light absorption properties,promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO_(2) molecules.The metal Co^(2+) at the center of the porphyrin molecules also acts as adsorption center for CO_(2) molecules,accelerating the CO_(2) conversion into CO and CH_(4).The possible mechanism of CO_(2) photoreduction was explored by in-situ FT-IR spectra.This work offers a new possibility for the preparation of advanced photocatalysts.展开更多
The establishment of S-scheme heterojunctions has arisen as a promising strategy for the advancement of efficient photocatalytic systems with superior charge separation and redox ability,specifically for H_(2)O_(2)pro...The establishment of S-scheme heterojunctions has arisen as a promising strategy for the advancement of efficient photocatalytic systems with superior charge separation and redox ability,specifically for H_(2)O_(2)production.In this investigation,an innovative 2D/2D g-C_(3)N_(4)/BiOBr S-scheme heterojunction was meticulously engineered through an in situ growth methodology.The synthetic composites exhibit boosted H_(2)O_(2)production activity,achieving a peak generation rate of 392μmol L^(-1)h^(-1),approximately 8.7-fold and 2.1-fold increase over the pristine BiOBr and g-C_(3)N_(4),respectively.Such a superior activity should be attributed to the highly efficient charge separation and migration mechanisms,along with the sustained robust redox capability of S-scheme heterostructure,which are verified by time-resolved photoluminescence spectroscopy,photocurrent test and electron paramagnetic resonance measurements.Furthermore,the interfacial electric field induced S-scheme charge transfer mechanism between g-C_(3)N_(4)and BiOBr is systematically certificated by in situ irradiated X-ray photoelectron spectroscopy and density functional theory calculation.This research offers a comprehensive protocol for the systematic development and construction of highly efficient S-scheme heterojunction photocatalysts,specifically tailored for enhanced H_(2)O_(2)production.展开更多
A Co_(3)O_(4)/BiOBr heterojunction was synthesized via a facile one-step solvothermal method for highly selec-tive photocatalytic CO_(2)reduction.The optimized Co_(3)O_(4)/BiOBr-0.8 catalyst exhibited CO and CH_(4)evo...A Co_(3)O_(4)/BiOBr heterojunction was synthesized via a facile one-step solvothermal method for highly selec-tive photocatalytic CO_(2)reduction.The optimized Co_(3)O_(4)/BiOBr-0.8 catalyst exhibited CO and CH_(4)evolution rates of 112.2 and 5.5µmol·g^(-1)·h^(-1),respectively,representing 6.3-fold and 3.9-fold enhancements over pristine BiOBr.The heterojunction demonstrated broadened light absorption,enhanced photoelectrochemical activity,reduced charge-transfer resistance,and improved separation efficiency of photogenerated carriers(e^(-)/h^(+)).These synergistic effects were attributed to the formation of a Z-scheme heterostructure,which facilitated solar energy utilization and electron reduction capacity while suppressing carrier recombination.展开更多
基金Supported by the National Natural Science Foundation of China(21978196)Natural Science Foundation of Shanxi Province(201801D211008,202403021211018)+1 种基金Shanxi Provincial Education Department(S202413597023)Jincheng High Efficiency Conversion and Utilization Technology Innovation Center of CO2 Energy and Biomass Energy。
文摘This study presents the successful synthesis of a novel Z-scheme heterojunction composite film consisting of Ag/Bi_(2)MoO_(6)/BiOBr through electrochemical processes and ionexchange techniques,followed by the photodeposition of noble metal silver(Ag)onto the composite structure.The catalytic efficiency of semiconductor photocatalysts is greatly improved by utilizing the localized surface plasmon resonance(LSPR)effect observed in Ag nanoparticles(NPs).Furthermore,the noble metal Ag serves as an intermediary bridge facilitating charge transfer between Bi_(2)MoO_(6)and BiOBr,while the formation of a Schottky barrier effectively inhibits the recombination of photo-generated electron-hole pairs.As a result,the Ag-deposited Bi_(2)MoO_(6)/BiOBr film exhibits superior photocatalytic performance in the reduction of CO_(2)compared to its unmodified counterpart.Our experimental results indicate a non-linear relationship between Ag deposition and the efficiency of photocatalytic CO_(2)reduction to CO,characterized by an initial increase in efficiency followed by a decline.The optimized 1.5%-Ag/Bi_(2)MoO_(6)/BiOBr film demonstrates exceptional photocatalytic activity,attaining a CO production rate of 13.65μmol/(g·h).This research explores the fundamental mechanisms that lead to improved photocatalytic CO_(2)reduction capabilities of the Ag/Bi_(2)MoO_(6)/BiOBr film.Our research offers important perspectives for the thoughtful design and production of highly efficient photocatalysts,which are essential for advancing sustainable energy solutions.
基金supported by the National Natural Science Foundation of China (No.52370174)the Natural Science Foundation of Shandong Province,China (No.ZR2022ME128)Special Projects in Key Areas of Colleges and Universities in Guangdong Province (No.2023ZDZX4050)。
文摘The excessive use of pesticides has exacerbated environmental pollution due to herbicide residues,while their persistent toxicity poses serious challenges to global ecological security.A magnetically recyclable CoFe_(2)O_(4)/BiOBr S-scheme heterojunctions was prepared by microwave-assisted co-precipitation method for photocatalytic degradation of Diuron(DUR) in water.The formation of S-scheme heterojunction enhances electron transfer and charge separation,which was demonstrated by free radical trapping,electrochemical experiments,and DFT calculations.The magnetic CoFe_(2)O_(4)/BiOBr catalysts can achieve 99.9 %removal of diuron in 50 min under visible light irradiation.Furthermore,the system maintains stable performance across a broad p H range(3-9),enabling adaptation to diverse water environments,effective elimination of multiple pollutants,and strong resistance to ionic interference.Using magnetic recovery,CoFe_(2)O_(4)/BiOBr exhibits a high removal rate of 99 % and a markedly low ion leaching rate(<20 μg/L) after six cycles photocatalytic process,confirming its excellent stability and durability.According to HPLCQTOF-MS and DFT calculation,the main ways of DUR degradation include dechlorinated hydroxylation,dealkylation and hydroxylation of aromatic ring and side chain.Toxicity analysis showed that the toxicity of the intermediates generated during degradation was generally lower than that of DUR.The magnetic CoFe_(2)O_(4)/BiOBr S-scheme heterojunction developed in this study exhibits excellent photocatalytic performance,high applicability,good stability,and durability,providing an effective magnetic for the removal of refractory pollutants.
基金financially supported by National Natural Science Foundation of China(Nos.22138011,22108106 and 22108108)China Postdoctoral Science Foundation(Nos.2022M721380 and 2020M680065)Hong Kong Scholar Program(XJ2021021).
文摘CO_(2) photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse effect.Herein,the 5,10,15,20-tetra(4-carboxyphenyl)porphyrin cobalt(II)(CoTCPP)has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr composite.The as-prepared CoTCPP/BiOBr-2 composite shows optimized photocatalytic performance for CO_(2) conversion into CO and CH_(4) upon irradiation with 300 W Xe lamp,which is 2.03 and 2.58 times compared to that of BiOBr,respectively.The introduced CoTCPP significantly enhanced light absorption properties,promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO_(2) molecules.The metal Co^(2+) at the center of the porphyrin molecules also acts as adsorption center for CO_(2) molecules,accelerating the CO_(2) conversion into CO and CH_(4).The possible mechanism of CO_(2) photoreduction was explored by in-situ FT-IR spectra.This work offers a new possibility for the preparation of advanced photocatalysts.
文摘The establishment of S-scheme heterojunctions has arisen as a promising strategy for the advancement of efficient photocatalytic systems with superior charge separation and redox ability,specifically for H_(2)O_(2)production.In this investigation,an innovative 2D/2D g-C_(3)N_(4)/BiOBr S-scheme heterojunction was meticulously engineered through an in situ growth methodology.The synthetic composites exhibit boosted H_(2)O_(2)production activity,achieving a peak generation rate of 392μmol L^(-1)h^(-1),approximately 8.7-fold and 2.1-fold increase over the pristine BiOBr and g-C_(3)N_(4),respectively.Such a superior activity should be attributed to the highly efficient charge separation and migration mechanisms,along with the sustained robust redox capability of S-scheme heterostructure,which are verified by time-resolved photoluminescence spectroscopy,photocurrent test and electron paramagnetic resonance measurements.Furthermore,the interfacial electric field induced S-scheme charge transfer mechanism between g-C_(3)N_(4)and BiOBr is systematically certificated by in situ irradiated X-ray photoelectron spectroscopy and density functional theory calculation.This research offers a comprehensive protocol for the systematic development and construction of highly efficient S-scheme heterojunction photocatalysts,specifically tailored for enhanced H_(2)O_(2)production.
文摘A Co_(3)O_(4)/BiOBr heterojunction was synthesized via a facile one-step solvothermal method for highly selec-tive photocatalytic CO_(2)reduction.The optimized Co_(3)O_(4)/BiOBr-0.8 catalyst exhibited CO and CH_(4)evolution rates of 112.2 and 5.5µmol·g^(-1)·h^(-1),respectively,representing 6.3-fold and 3.9-fold enhancements over pristine BiOBr.The heterojunction demonstrated broadened light absorption,enhanced photoelectrochemical activity,reduced charge-transfer resistance,and improved separation efficiency of photogenerated carriers(e^(-)/h^(+)).These synergistic effects were attributed to the formation of a Z-scheme heterostructure,which facilitated solar energy utilization and electron reduction capacity while suppressing carrier recombination.
