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
Proper design and preparation of high-performance and stable dual functional photocatalytic materials remains a significant objective of research. In this work, highly dispersed noble-metal nanoparticles （Au, Pd, Pt...Proper design and preparation of high-performance and stable dual functional photocatalytic materials remains a significant objective of research. In this work, highly dispersed noble-metal nanoparticles （Au, Pd, Pt） were immobilized on MIL-100（Fe） （denoted M@MIL-100（Fe）） using a facile room-temperature photodeposition technique. The resulting M@MIL-100（Fe） （M = Au, Pd, and Pt） nanocomposites exhibited enhanced photoactivities toward photocatalytic degradation of methyl orange （MO） and reduction of heavy-metal Cr（VI） ions under visible-light irradiation （A ≥ 420 nm） compared with blank-MIL-100（Fe）. Combining these results with photoelectrochemical analyses revealed that noble-metal deposition can effectively improve the charge-separation efficiency of MIL-100（Fe） under visible-light irradiation. This phenomenon in turn leads to the enhancement of visible-light-driven photoactivity of M@MIL-100（Fe） toward photocatalytic redox reactions. In particular, the Pt@MIL-100（Fe） with an average Pt particle size of 2 nm exhibited remarkably enhanced photoactivities compared with those of M@MIL-100（Fe） （M = Au and Pd）, which can be attributed to the integrative effect of the enhanced light absorption intensity and more efficient separation of the photogenerated charge carrier. In addition, possible photocatalytic reaction mechanisms are also proposed.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This work was supported by the National Natural Science Foundation of China （Nos. 21273036 and 21177024） and Science ＆ Technology Plan Project of Fujian Province （No. 2014Y2003）.
文摘Proper design and preparation of high-performance and stable dual functional photocatalytic materials remains a significant objective of research. In this work, highly dispersed noble-metal nanoparticles （Au, Pd, Pt） were immobilized on MIL-100（Fe） （denoted M@MIL-100（Fe）） using a facile room-temperature photodeposition technique. The resulting M@MIL-100（Fe） （M = Au, Pd, and Pt） nanocomposites exhibited enhanced photoactivities toward photocatalytic degradation of methyl orange （MO） and reduction of heavy-metal Cr（VI） ions under visible-light irradiation （A ≥ 420 nm） compared with blank-MIL-100（Fe）. Combining these results with photoelectrochemical analyses revealed that noble-metal deposition can effectively improve the charge-separation efficiency of MIL-100（Fe） under visible-light irradiation. This phenomenon in turn leads to the enhancement of visible-light-driven photoactivity of M@MIL-100（Fe） toward photocatalytic redox reactions. In particular, the Pt@MIL-100（Fe） with an average Pt particle size of 2 nm exhibited remarkably enhanced photoactivities compared with those of M@MIL-100（Fe） （M = Au and Pd）, which can be attributed to the integrative effect of the enhanced light absorption intensity and more efficient separation of the photogenerated charge carrier. In addition, possible photocatalytic reaction mechanisms are also proposed.
