With the growing concern about the water environment,the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutan...With the growing concern about the water environment,the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutants.In this work,to overcome the drawbacks of the photocatalytic activity reduction caused by the photo-corrosion of non-stoichiometric BiO_(2–x),a novel material with amorphous FeOOH in situ grown on layered BiO_(2–x) to form a core-shell structure similar to popcorn chicken-like morphology was produced in two simple and environmentally beneficial steps.Through a series of degradation activity tests of hybrid materials under different conditions,the as-prepared materials exhibited remarkable degradation activity and stability toward tetracycline in the FeOOH@BiO_(2–x)/Vis/PS system due to the synergism of photocatalysis and persulfate activation.The results of XRD,SEM,TEM,XPS,FTIR,and BET show that the loading of FeOOH increases the specific surface area and active sites appreciably;the heterogeneous structure formed by FeOOH and BiO_(2–x) is more favorable to the effective separation of photogenerated carriers.The optimal degradation conditions were at a catalyst addition of 0.7 g·L^(–1),a persulfate concentration of 1.0 g·L^(–1),and an initial pH of 4.5,at which the degradation rate could reach 94.7%after 90 min.The influence of typical inorganic anions on degradation was also examined.ESR studies and radical quenching experiments revealed that·OH,SO_(4)^(-)·,and·O_(2)^(-)were the principal active species generated during the degradation of tetracycline.The results of the 1,10-phenanthroline approach proved that the effect of dissolved iron ions on the tetracycline degradation was limited,and the interfacial reaction that occurs on the active sites on the material's surface was a critical factor.This work provides a novel method for producing efficient broad-spectrum Bismuth-based composite photocatalysts and photocatalytic-activated persulfate synergistic degradation of tetracycline.展开更多
The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)...The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.展开更多
基金supported by the National Key Research and Development Program of China(2019YFC1904100)the National Natural Science Foundation of China(21503144)+3 种基金the Science and Technology Innovation Project for Students of Hebei Province(22E50174D)the Science and Technology Project of Hebei Education Department(QN2021047)the Program of Hebei Vocational University of Industry and Technology(dxs202207,ZY202401)the Key Program of Natural Science of Hebei Province(B2020209017).
文摘With the growing concern about the water environment,the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutants.In this work,to overcome the drawbacks of the photocatalytic activity reduction caused by the photo-corrosion of non-stoichiometric BiO_(2–x),a novel material with amorphous FeOOH in situ grown on layered BiO_(2–x) to form a core-shell structure similar to popcorn chicken-like morphology was produced in two simple and environmentally beneficial steps.Through a series of degradation activity tests of hybrid materials under different conditions,the as-prepared materials exhibited remarkable degradation activity and stability toward tetracycline in the FeOOH@BiO_(2–x)/Vis/PS system due to the synergism of photocatalysis and persulfate activation.The results of XRD,SEM,TEM,XPS,FTIR,and BET show that the loading of FeOOH increases the specific surface area and active sites appreciably;the heterogeneous structure formed by FeOOH and BiO_(2–x) is more favorable to the effective separation of photogenerated carriers.The optimal degradation conditions were at a catalyst addition of 0.7 g·L^(–1),a persulfate concentration of 1.0 g·L^(–1),and an initial pH of 4.5,at which the degradation rate could reach 94.7%after 90 min.The influence of typical inorganic anions on degradation was also examined.ESR studies and radical quenching experiments revealed that·OH,SO_(4)^(-)·,and·O_(2)^(-)were the principal active species generated during the degradation of tetracycline.The results of the 1,10-phenanthroline approach proved that the effect of dissolved iron ions on the tetracycline degradation was limited,and the interfacial reaction that occurs on the active sites on the material's surface was a critical factor.This work provides a novel method for producing efficient broad-spectrum Bismuth-based composite photocatalysts and photocatalytic-activated persulfate synergistic degradation of tetracycline.
基金the funding support from the National Natural Science Foundation of China(21906072,22006057)the Natural Science Foundation of Jiangsu Province(BK20190982)“Doctor of Mass entrepreneurship and innovation”Project in Jiangsu Province。
文摘The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.
