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
Total dissolved nitrogen(TDN) is an important parameter for assessing the nutrient cycling and status of natural waters.The accurate determination of TDN in natural waters is essential for assessing its contents and d...Total dissolved nitrogen(TDN) is an important parameter for assessing the nutrient cycling and status of natural waters.The accurate determination of TDN in natural waters is essential for assessing its contents and distinguishing different forms of nitrogen in the water.The TDN in various systems has been largely documented,and the concentrations of TDN are usually obtained using high-temperature catalytic(HTC) or persulfate oxidation(PO).However,the accuracy of these methods and their suitability for all types of natural waters are still unclear.To explore both methods in-depth,assorted samples were tested,including eight solutions composed of nitrogen-containing compounds(3 dissolved inorganic nitrogen fractions:NO_(3)^(-),NO_(2)^(-)and NH_(4)^(+);5 organic compounds:EDTA-2Na,vitamin B1,vitamin B12,amino acids,and urea) and 105 natural waters which were collected from an open ocean(Northwest Pacific Ocean,28),a marginal sea(Yellow Sea,34),an estuary(Huanghe River mouth,31),rivers(Huanghe River,4;Licun River,4),and precipitations(4 samples).The results showed that heterocycles and molecular dimensions had certain effects on the oxidation efficiency of the PO method but had little effect on HTC.There was no significant difference between the two methods for natural waters,but HTC was more suitable for deep-sea samples with low TDN concentrations(less than 10 μmol/L) and low organic activity.Overall,HTC has a relatively simple measurement process,a high degree of automation,and low error.Therefore,HTC can be recommended to determine the TDN of samples in freshwater and seawater.展开更多
A synergistic system of water falling film dielectric barrier discharge(DBD)plasma and persulfate(PS)was set up and used for oxidizing ciprofloxacin(CIP)in water.Results of reactive species formation in the DBD-only s...A synergistic system of water falling film dielectric barrier discharge(DBD)plasma and persulfate(PS)was set up and used for oxidizing ciprofloxacin(CIP)in water.Results of reactive species formation in the DBD-only system as well as the DBD–PS system verified the PS activation in the DBD system.Influencing factors on CIP degradation and the degradation process were also been studied.The obtained results showed that the presence of PS could greatly improve the degradation and mineralization of CIP and that the degradation efficiency could reach 97.73%after only 40 min treatment with 4 m M PS addition.The increase of PS concentration,the lower CIP concentration,the acidic solution p H and the addition of metal ions(Fe^(2+)and Cu^(2+))enhanced the CIP degradation,while the existence of Cl^(-)and HCO_(3)^(-)had a negative effect.The experiments related to scavenger addition confirmed the contribution of the main reactive species to the CIP oxidation.Three probable degradation pathways were proposed by analyzing the inorganic ions and organic byproducts formed during the CIP degradation.The toxicity evaluation results of the CIP and its intermediates confirmed the effectiveness of the DBD–PS synergistic system.展开更多
Palladium(Pd)-based sulfides have triggered extensive interest due to their unique properties and potential applications in the fields of electronics and optoelectronics.However,the synthesis of large-scale uniform Pd...Palladium(Pd)-based sulfides have triggered extensive interest due to their unique properties and potential applications in the fields of electronics and optoelectronics.However,the synthesis of large-scale uniform PdS and PdS_(2)nanofilms(NFs)remains an enormous challenge.In this work,2-inch wafer-scale PdS and PdS_(2) NFs with excellent stability can be controllably prepared via chemical vapor deposition combined with electron beam evaporation technique.The thickness of the pre-deposited Pd film and the sulfurization temperature are critical for the precise synthesis of PdS and PdS_(2) NFs.A corresponding growth mechanism has been proposed based on our experimental results and Gibbs free energy calculations.The electrical transport properties of PdS and PdS_(2) NFs were explored by conductive atomic force microscopy.Our findings have achieved the controllable growth of PdS and PdS_(2) NFs,which may provide a pathway to facilitate PdS and PdS_(2) based applications for next-generation high performance optoelectronic devices.展开更多
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.
基金The National Key Research and Development Project of China under contract No.2019YFC1407802the Fund of State Environmental Protection Key Laboratory of Coastal Ecosystem under contract No.202112+3 种基金the Open Fund of Key Laboratory of Marine Ecological Environment Science and EngineeringMinistry of Natural Resources under contract No.MESE-2019-06the National Natural Science Foundation of China under contract No.41876078the Shandong Provincial Natural Science Foundation of China under contract No.ZR2018MD016。
文摘Total dissolved nitrogen(TDN) is an important parameter for assessing the nutrient cycling and status of natural waters.The accurate determination of TDN in natural waters is essential for assessing its contents and distinguishing different forms of nitrogen in the water.The TDN in various systems has been largely documented,and the concentrations of TDN are usually obtained using high-temperature catalytic(HTC) or persulfate oxidation(PO).However,the accuracy of these methods and their suitability for all types of natural waters are still unclear.To explore both methods in-depth,assorted samples were tested,including eight solutions composed of nitrogen-containing compounds(3 dissolved inorganic nitrogen fractions:NO_(3)^(-),NO_(2)^(-)and NH_(4)^(+);5 organic compounds:EDTA-2Na,vitamin B1,vitamin B12,amino acids,and urea) and 105 natural waters which were collected from an open ocean(Northwest Pacific Ocean,28),a marginal sea(Yellow Sea,34),an estuary(Huanghe River mouth,31),rivers(Huanghe River,4;Licun River,4),and precipitations(4 samples).The results showed that heterocycles and molecular dimensions had certain effects on the oxidation efficiency of the PO method but had little effect on HTC.There was no significant difference between the two methods for natural waters,but HTC was more suitable for deep-sea samples with low TDN concentrations(less than 10 μmol/L) and low organic activity.Overall,HTC has a relatively simple measurement process,a high degree of automation,and low error.Therefore,HTC can be recommended to determine the TDN of samples in freshwater and seawater.
基金National Natural Science Foundation of China(No.21876070)for their support of this study.
文摘A synergistic system of water falling film dielectric barrier discharge(DBD)plasma and persulfate(PS)was set up and used for oxidizing ciprofloxacin(CIP)in water.Results of reactive species formation in the DBD-only system as well as the DBD–PS system verified the PS activation in the DBD system.Influencing factors on CIP degradation and the degradation process were also been studied.The obtained results showed that the presence of PS could greatly improve the degradation and mineralization of CIP and that the degradation efficiency could reach 97.73%after only 40 min treatment with 4 m M PS addition.The increase of PS concentration,the lower CIP concentration,the acidic solution p H and the addition of metal ions(Fe^(2+)and Cu^(2+))enhanced the CIP degradation,while the existence of Cl^(-)and HCO_(3)^(-)had a negative effect.The experiments related to scavenger addition confirmed the contribution of the main reactive species to the CIP oxidation.Three probable degradation pathways were proposed by analyzing the inorganic ions and organic byproducts formed during the CIP degradation.The toxicity evaluation results of the CIP and its intermediates confirmed the effectiveness of the DBD–PS synergistic system.
基金supported by National Natural Science Foundation of China (No.11974301)Key Research and Development Program of Hunan Province (No.2022GK2007)+2 种基金Key Project from Department Education of Hunan Province (No.22A0123)Scientific Research Fund of Hunan Provincial Education Department (No.21B0136)National college students innovation and entrepreneurship training program (No.S202310530016)。
文摘Palladium(Pd)-based sulfides have triggered extensive interest due to their unique properties and potential applications in the fields of electronics and optoelectronics.However,the synthesis of large-scale uniform PdS and PdS_(2)nanofilms(NFs)remains an enormous challenge.In this work,2-inch wafer-scale PdS and PdS_(2) NFs with excellent stability can be controllably prepared via chemical vapor deposition combined with electron beam evaporation technique.The thickness of the pre-deposited Pd film and the sulfurization temperature are critical for the precise synthesis of PdS and PdS_(2) NFs.A corresponding growth mechanism has been proposed based on our experimental results and Gibbs free energy calculations.The electrical transport properties of PdS and PdS_(2) NFs were explored by conductive atomic force microscopy.Our findings have achieved the controllable growth of PdS and PdS_(2) NFs,which may provide a pathway to facilitate PdS and PdS_(2) based applications for next-generation high performance optoelectronic devices.
