Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mec...Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mechanism of arsenopyrite by evaluating the effects of physical and chemical changes of arsenopyrite in BOS chemical oxidation stage on mineral dissolution kinetics,as well as microbial growth activity and community structure composition in bio-oxidation stage.The results showed that the chemical oxidation contributed to destroying the physical and chemical structure of arsenopyrite surface and reducing the particle size,and led to the formation of nitrogenous substances on mineral surface.These chemical oxidation behaviors effectively promoted Fe^(3+)cycling in the bio-oxidation system and weakened the inhibitory effect of the sulfur film on ionic diffusion,thereby enhancing the dissolution kinetics of the arsenopyrite.Therefore,the bio-oxidation efficiency of arsenopyrite was significantly increased in the two-stage oxidation process.After 18 d,the two-stage oxidation process achieved total extraction rates of(88.8±2.0)%,(86.7±1.3)%,and(74.7±3.0)%for As,Fe,and S elements,respectively.These values represented a significant increase of(50.8±3.4)%,(47.1±2.7)%,and(46.0±0.7)%,respectively,compared to the one-stage bio-oxidation process.展开更多
Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for d...Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.展开更多
Sulfur removal from liquid fuels has increased in importance in recent years. Although hydrodesulfurization is the usual method for removing sulfur, the elimination of thiophene compounds using this process is difficu...Sulfur removal from liquid fuels has increased in importance in recent years. Although hydrodesulfurization is the usual method for removing sulfur, the elimination of thiophene compounds using this process is difficult. Photocatalysis is an alternative method being developed for thiophene removal at ambient conditions. Among semiconductors, titania has shown good potential as a photo-catalyst; however, quick recombination of electron holes hinders its commercial use. One way to decrease the recombination rate is to combine carbon nanotubes with a semiconductor. In this work, multiwall carbon nanotube （MWCNT） / titania composites were prepared with different mass ratios of MWCNT to titania using tetraethyl orthotitanate （TEOT） and titanium tetra isopropoxide （TTIP） as precursors of titania. Dibenzothiophene （DBT） photocatalytic removal from n-hexane was measured in both the presence and absence of oxygen. The results indicated that the best removal occurred when the MWCNT to titania ratio was 1. When the ratio exceeded this number, DBT removal efficiency decreased due to light scattering. Also, the composites prepared by TEOT exhibited better efficiency in DBT removal. The research findings suggested that the obtained composite was a visible light active photocatalyst and exhibited better performance in the presence of oxygen. Kinetics of photocatalytic DBT removal was a first-order reaction with removal rate constant 0.7 h–1 obtained at optimum conditions.展开更多
Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laborat...Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laboratory-scale reactor. Effects of several key operational parameters on NO removal efficiency are studied, including TiO2 content, H2O2 initial concentration, UV lamp power, NO initial content, oxygen volume fraction and TiO2/H2O2 solution volume. The results illustrate that the NO removal efficiency increases with the increasing of H2O2 initial concentration or UV lamp power. Meanwhile, a lower NO initial content or a higher TiO2/H2O2 solution volume will result in higher NO removal efficiency. In addition, oxygen volume fraction has a little effect.The highest NO removal efficiency is achieved at the TiO2 content of 0.75 g/L, H2O2 initial concentration of 2.5 mol/L, UV lamp power of 36 W, NO initial content of 206×10-6 and TiO2/H2O2 solution volume of 600 m L. It is beneficial for the development and application of NO removal from coal-fired flue gas with UV/TiO2/H2O2 process.展开更多
In the present work, a novel heterogeneous photo-Fenton catalyst was prepared by iron and cerium pillared bentonite. The catalyst Fe-Ce/bentonite was characterized by X-ray diffraction （XRD）, X-ray fluorescence （XR...In the present work, a novel heterogeneous photo-Fenton catalyst was prepared by iron and cerium pillared bentonite. The catalyst Fe-Ce/bentonite was characterized by X-ray diffraction （XRD）, X-ray fluorescence （XRF）, Brunauer-Emmett-Teller （BET） and scanning electron microscopy （SEM） methods. It is found that Fe and Ce intercalate into the silicate layers of bentonite successfully. Tetracycline was removed by heterogeneous photo-Fenton reaction using the catalyst in this work. The effects of different reaction systems, hydrogen peroxide concentration, initial pH, catalyst dosage, UV power and introduction of different anions on degradation were investigated in details. The stability of catalyst was investigated through recycling experiment. The results show that removal rate of tetracycline is 98.13% under the conditions of 15 mmol/L H202, 0.50 g/L catalyst dosage, initial pH 3.0, 11 W UV lamp power and 60 min reaction time. However, the removal rate decreases after adding some anions. The hydroxyl radical plays an important role in heterogeneous photo-assisted Fenton degradation of tetracycline. The catalyst is very stable and can be recycled many times.展开更多
Natural minerals receive growing attention as inexpensive, green, and efficient catalysts for degradation of organic pollutants. Mechanical activation of natural chalcopyrite was conducted for improving the catalytic ...Natural minerals receive growing attention as inexpensive, green, and efficient catalysts for degradation of organic pollutants. Mechanical activation of natural chalcopyrite was conducted for improving the catalytic performance.Tetracycline degradation was evaluated in the presence of hydrogen peroxide and mechanically activated chalcopyrite.Tetracycline degradation at 100 min is 55.52%(Chp10), 68.97%(Chp30), 77.79%(Chp60), and 86.43%(Chp120),respectively, and the rate constant of pseudo-first-order kinetics is 0.0079, 0.0109, 0.0137 and 0.0192 min^(-1), respectively.Chalcopyrite samples were examined by multiple characterizations. Mechanical activation of natural chalcopyrite induces the decline of particle size and slight increase of surface area, smaller grain size, lattice strain, and partial sulfur oxidation. The relationship between catalytic activity and property change manifests that the improved catalytic ability is mainly ascribed to the increase of surface area and surface oxidation induced by mechanical activation. This work provides novel insights into the improvement of catalytic performance of natural minerals by mechanical activation.展开更多
Decoloration and mineralization of yeast wastewater were investigated by using Ce-Fe/Al2O3 as a heterogeneous photo-Fenton catalyst in fluidized bed reactor in order to solve the problem of yeast wastewater discharge....Decoloration and mineralization of yeast wastewater were investigated by using Ce-Fe/Al2O3 as a heterogeneous photo-Fenton catalyst in fluidized bed reactor in order to solve the problem of yeast wastewater discharge. The experimental results were assessed in terms of total organic carbon（TOC） reduction. The operational and reaction conditions affecting the efficiencies of TOC removal such as initial pH value, H2O2 concentration, catalyst loading and UV power were studied. The results show that TOC is reduced from 347.6 mg/L to 10.8 mg/L, color is changed from 500 units to 0 under the conditions as follows： initial pH value 6. 0, H2O2 concentration of 1. 000 g/L, catalyst loading of 5 g/L, reaction duration of 120 rain and reaction temperature of 30 ℃. The irradiated Ce-Fe/Al2O3 catalyst was complexed with 1,10-phenanthroline and then it was subjected to Fourier transform infrared spectroscopy and diffuse reflectance spectroscopy to confirm the formation of Fe（Ⅱ） in the solid state. Heterogeneous photo-Fenton reaction proves to be effective for the treatment of yeast wastewater.展开更多
基金Project(52274348)supported by the National Natural Science Foundation of ChinaProject(2022JH1/10400024)supported by the Major Projects for the“Revealed Top”Science and Technology of Liaoning Province,China。
文摘Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mechanism of arsenopyrite by evaluating the effects of physical and chemical changes of arsenopyrite in BOS chemical oxidation stage on mineral dissolution kinetics,as well as microbial growth activity and community structure composition in bio-oxidation stage.The results showed that the chemical oxidation contributed to destroying the physical and chemical structure of arsenopyrite surface and reducing the particle size,and led to the formation of nitrogenous substances on mineral surface.These chemical oxidation behaviors effectively promoted Fe^(3+)cycling in the bio-oxidation system and weakened the inhibitory effect of the sulfur film on ionic diffusion,thereby enhancing the dissolution kinetics of the arsenopyrite.Therefore,the bio-oxidation efficiency of arsenopyrite was significantly increased in the two-stage oxidation process.After 18 d,the two-stage oxidation process achieved total extraction rates of(88.8±2.0)%,(86.7±1.3)%,and(74.7±3.0)%for As,Fe,and S elements,respectively.These values represented a significant increase of(50.8±3.4)%,(47.1±2.7)%,and(46.0±0.7)%,respectively,compared to the one-stage bio-oxidation process.
基金University Synergy Innovation Program of Anhui Province(GXXT-2022-083)Science and Technology Plan Project of Wuhu City,China(2023kx12)Anhui Provincial Department of Education New Era Education Project(2023xscx070)。
文摘Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.
文摘Sulfur removal from liquid fuels has increased in importance in recent years. Although hydrodesulfurization is the usual method for removing sulfur, the elimination of thiophene compounds using this process is difficult. Photocatalysis is an alternative method being developed for thiophene removal at ambient conditions. Among semiconductors, titania has shown good potential as a photo-catalyst; however, quick recombination of electron holes hinders its commercial use. One way to decrease the recombination rate is to combine carbon nanotubes with a semiconductor. In this work, multiwall carbon nanotube （MWCNT） / titania composites were prepared with different mass ratios of MWCNT to titania using tetraethyl orthotitanate （TEOT） and titanium tetra isopropoxide （TTIP） as precursors of titania. Dibenzothiophene （DBT） photocatalytic removal from n-hexane was measured in both the presence and absence of oxygen. The results indicated that the best removal occurred when the MWCNT to titania ratio was 1. When the ratio exceeded this number, DBT removal efficiency decreased due to light scattering. Also, the composites prepared by TEOT exhibited better efficiency in DBT removal. The research findings suggested that the obtained composite was a visible light active photocatalyst and exhibited better performance in the presence of oxygen. Kinetics of photocatalytic DBT removal was a first-order reaction with removal rate constant 0.7 h–1 obtained at optimum conditions.
基金Project(2011CB201505)supported by the National Key Basic Research Program of ChinaProject(BA2011031)supported by the Special Fund of Transformation of Scientific and Technological Achievements of Jiangsu Province,China
文摘Nitric oxide(NO) from flue gas is hard to remove because of low solubility and reactivity. A new technology for photocatalytic oxidation of NO using ultraviolet(UV)/TiO2/H2O2 process is studied in an efficient laboratory-scale reactor. Effects of several key operational parameters on NO removal efficiency are studied, including TiO2 content, H2O2 initial concentration, UV lamp power, NO initial content, oxygen volume fraction and TiO2/H2O2 solution volume. The results illustrate that the NO removal efficiency increases with the increasing of H2O2 initial concentration or UV lamp power. Meanwhile, a lower NO initial content or a higher TiO2/H2O2 solution volume will result in higher NO removal efficiency. In addition, oxygen volume fraction has a little effect.The highest NO removal efficiency is achieved at the TiO2 content of 0.75 g/L, H2O2 initial concentration of 2.5 mol/L, UV lamp power of 36 W, NO initial content of 206×10-6 and TiO2/H2O2 solution volume of 600 m L. It is beneficial for the development and application of NO removal from coal-fired flue gas with UV/TiO2/H2O2 process.
基金Project(51004053)supported by National Natural Science Foundation of ChinaProject(2009J01033)supported by Natural Science Foundation of Fujian Province,China+2 种基金Project(3502Z20116008)supported by the Science and Technology Research Project of Xiamen City,ChinaProject(JA11146)supported by Program for Fostering Distinguished Young Scholars in University of Fujian Province,ChinaProject(2011B003)supported by the Foundation for Young Professors of Jimei University,China
文摘In the present work, a novel heterogeneous photo-Fenton catalyst was prepared by iron and cerium pillared bentonite. The catalyst Fe-Ce/bentonite was characterized by X-ray diffraction （XRD）, X-ray fluorescence （XRF）, Brunauer-Emmett-Teller （BET） and scanning electron microscopy （SEM） methods. It is found that Fe and Ce intercalate into the silicate layers of bentonite successfully. Tetracycline was removed by heterogeneous photo-Fenton reaction using the catalyst in this work. The effects of different reaction systems, hydrogen peroxide concentration, initial pH, catalyst dosage, UV power and introduction of different anions on degradation were investigated in details. The stability of catalyst was investigated through recycling experiment. The results show that removal rate of tetracycline is 98.13% under the conditions of 15 mmol/L H202, 0.50 g/L catalyst dosage, initial pH 3.0, 11 W UV lamp power and 60 min reaction time. However, the removal rate decreases after adding some anions. The hydroxyl radical plays an important role in heterogeneous photo-assisted Fenton degradation of tetracycline. The catalyst is very stable and can be recycled many times.
基金Project(2020YFC1908802) supported by the National Key Research and Development Project of China。
文摘Natural minerals receive growing attention as inexpensive, green, and efficient catalysts for degradation of organic pollutants. Mechanical activation of natural chalcopyrite was conducted for improving the catalytic performance.Tetracycline degradation was evaluated in the presence of hydrogen peroxide and mechanically activated chalcopyrite.Tetracycline degradation at 100 min is 55.52%(Chp10), 68.97%(Chp30), 77.79%(Chp60), and 86.43%(Chp120),respectively, and the rate constant of pseudo-first-order kinetics is 0.0079, 0.0109, 0.0137 and 0.0192 min^(-1), respectively.Chalcopyrite samples were examined by multiple characterizations. Mechanical activation of natural chalcopyrite induces the decline of particle size and slight increase of surface area, smaller grain size, lattice strain, and partial sulfur oxidation. The relationship between catalytic activity and property change manifests that the improved catalytic ability is mainly ascribed to the increase of surface area and surface oxidation induced by mechanical activation. This work provides novel insights into the improvement of catalytic performance of natural minerals by mechanical activation.
基金Project(20277010) supported by the National Natural Science Foundation of China
文摘Decoloration and mineralization of yeast wastewater were investigated by using Ce-Fe/Al2O3 as a heterogeneous photo-Fenton catalyst in fluidized bed reactor in order to solve the problem of yeast wastewater discharge. The experimental results were assessed in terms of total organic carbon（TOC） reduction. The operational and reaction conditions affecting the efficiencies of TOC removal such as initial pH value, H2O2 concentration, catalyst loading and UV power were studied. The results show that TOC is reduced from 347.6 mg/L to 10.8 mg/L, color is changed from 500 units to 0 under the conditions as follows： initial pH value 6. 0, H2O2 concentration of 1. 000 g/L, catalyst loading of 5 g/L, reaction duration of 120 rain and reaction temperature of 30 ℃. The irradiated Ce-Fe/Al2O3 catalyst was complexed with 1,10-phenanthroline and then it was subjected to Fourier transform infrared spectroscopy and diffuse reflectance spectroscopy to confirm the formation of Fe（Ⅱ） in the solid state. Heterogeneous photo-Fenton reaction proves to be effective for the treatment of yeast wastewater.
