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
MIL-101(Cr)is a promising moisture absorbent for solar-driven water harvesting from moisture to tackle the worldwide water shortage issue.However,the MIL-101(Cr)powder suffers from a long ab/desorption cycle due to th...MIL-101(Cr)is a promising moisture absorbent for solar-driven water harvesting from moisture to tackle the worldwide water shortage issue.However,the MIL-101(Cr)powder suffers from a long ab/desorption cycle due to the crystal aggregation caused by its inherent powder properties.Here,we demonstrate a MIL-101(Cr)nanofibrous composite membrane with a nanofibrous matrix where MIL-101(Cr)is monodisperse in the 3D porous nanofibrous matrix through a simple spray-electrospinning strategy.The continuous porous nanofibrous matrix not only offers sufficient sites for MIL-101(Cr)loading but also provides rapid moisture transport channels,resulting in a super-rapid ab/desorption duration of 50 min(including an absorption process for 40 min and a desorption process for 10 min)and multicycle daily water production of 15.9 L kg^(−1) d^(−1).Besides,the MIL-101(Cr)nanofibrous composite membrane establishes a high solar absorption of 92.8%,and excellent photothermal conversion with the surface temperature of 70.7°C under one-sun irradiation.In addition,the MIL-101(Cr)nanofibrous composite membrane shows excellent potential for practical application due to its flexibility,portability,and use stability.This work provides a new perspective of shortening MOF ab/desorption duration by introducing a porous nanofibrous matrix to improve the specific water production for the solar-driven ab/desorption water harvesting technique.展开更多
In this work, a series of MIL-101-SO3H(x) polymeric materials were prepared and further used for the first time as efficient heterogeneous catalysts for the conversion of fructose-based carbohydrates into 5-ethoxyme...In this work, a series of MIL-101-SO3H(x) polymeric materials were prepared and further used for the first time as efficient heterogeneous catalysts for the conversion of fructose-based carbohydrates into 5-ethoxymethylfurfural(EMF) in a renewable mixed solvent system consisting of ethanol and tetrahydrofuran(THF). The influence of –SO3H content on the acidity as well as on the catalytic activity of the porous coordination polymers in EMF production was also studied. High EMF yields of 67.7% and 54.2% could be successively obtained from fructose and inulin in the presence of MIL-101-SO;H(100) at 130 °C for 15 h.The catalyst could be reused for five times without significant loss of its activity and the recovery process was facile and simple. This work provides a new platform by application of porous coordination polymers(PCPs) for the production of the potential liquid fuel molecule EMF from biomass in a sustainable solvent system.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 partly supported by the Funda-mental Research Funds for the Central Universi-ties (2232020D-15,2232020A-08,2232020G-01,2232020D-14,and 2232019D3-11)grants (51773037,51973027,51803023,52003044,and 61771123)from the National Natural Science Foundation of China+3 种基金This work has also been supported by the Chang Jiang Scholars Program and the Innovation Program of Shanghai Munici-pal Education Commission (2019-01-07-00-03-E00023)to Prof.Xiaohong Qinthe Shanghai Sailing Program (19YF1400700)the Opening Project of State Key Laboratory of High-Performance Ceramics and Superfine Microstruc-ture (SKL201906SIC)Young Elite Scientists Sponsorship Program by CAST and DHU Distin-guished Young Professor Program to Prof.Liming Wang.
文摘MIL-101(Cr)is a promising moisture absorbent for solar-driven water harvesting from moisture to tackle the worldwide water shortage issue.However,the MIL-101(Cr)powder suffers from a long ab/desorption cycle due to the crystal aggregation caused by its inherent powder properties.Here,we demonstrate a MIL-101(Cr)nanofibrous composite membrane with a nanofibrous matrix where MIL-101(Cr)is monodisperse in the 3D porous nanofibrous matrix through a simple spray-electrospinning strategy.The continuous porous nanofibrous matrix not only offers sufficient sites for MIL-101(Cr)loading but also provides rapid moisture transport channels,resulting in a super-rapid ab/desorption duration of 50 min(including an absorption process for 40 min and a desorption process for 10 min)and multicycle daily water production of 15.9 L kg^(−1) d^(−1).Besides,the MIL-101(Cr)nanofibrous composite membrane establishes a high solar absorption of 92.8%,and excellent photothermal conversion with the surface temperature of 70.7°C under one-sun irradiation.In addition,the MIL-101(Cr)nanofibrous composite membrane shows excellent potential for practical application due to its flexibility,portability,and use stability.This work provides a new perspective of shortening MOF ab/desorption duration by introducing a porous nanofibrous matrix to improve the specific water production for the solar-driven ab/desorption water harvesting technique.
基金financially supported by the Natural Science Foundation of China(no.21576059)the Key Technologies R&D Program(no.2011BAE06B02)+1 种基金the International Science&Technology Cooperation Program of China(2010DFB60840)the Science and Technology Project of Guizhou Province(nos.[2012]6012 and[2011]3016)
文摘In this work, a series of MIL-101-SO3H(x) polymeric materials were prepared and further used for the first time as efficient heterogeneous catalysts for the conversion of fructose-based carbohydrates into 5-ethoxymethylfurfural(EMF) in a renewable mixed solvent system consisting of ethanol and tetrahydrofuran(THF). The influence of –SO3H content on the acidity as well as on the catalytic activity of the porous coordination polymers in EMF production was also studied. High EMF yields of 67.7% and 54.2% could be successively obtained from fructose and inulin in the presence of MIL-101-SO;H(100) at 130 °C for 15 h.The catalyst could be reused for five times without significant loss of its activity and the recovery process was facile and simple. This work provides a new platform by application of porous coordination polymers(PCPs) for the production of the potential liquid fuel molecule EMF from biomass in a sustainable solvent system.