Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex(Fe(III)-Ox).The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-...Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex(Fe(III)-Ox).The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-Ox under solar irradiation.Although the photolysis mechanisms of Fe(III)-Ox have been investigated extensively,information about the oxidation of volatile organic compounds(VOC),specifically the potential for Secondary Organic Aerosol(SOA)formation in the Fe(III)-Ox system,is lacking.In this study,a ubiquitous VOC methacrolein(MACR)is chosen as a model VOC,and the oxidation of MACR with Fe(III)-Ox is investigated under typical atmospheric water conditions.The effects of oxalate concentration,Fe(III)concentration,MACR concentration,and pH on the oxidation of MACR are studied in detail.Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(III).The oxidation rate of MACR also accelerates with increasing concentration of oxalate.The effect of Fe(III)is found to be more complicated.The oxidation rate of MACR first increases and then decreases with increasing Fe(III)concentration.The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration.The production of ferrous and hydrogen peroxide,pH,and aqueous absorbance are monitored throughout the reaction process.The quenching experiments verify that·OH and O_(2)^(+)are both responsible for the oxidation of MACR.MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight,which contributes to the yield of SOA.These results suggest that Fe(III)-Ox plays an important role in atmospheric oxidation.展开更多
Battery grade γ-MnO2 powder was investigated as an oxidant and an adsorbent in combination with Fe/Al coagulants for removal of arsenic from contaminated water. Simultaneous oxidation of As(III) and removal by coprec...Battery grade γ-MnO2 powder was investigated as an oxidant and an adsorbent in combination with Fe/Al coagulants for removal of arsenic from contaminated water. Simultaneous oxidation of As(III) and removal by coprecipitation/adsorption (one step process) was compared with pre-oxidation and subsequent removal by coprecipitation/adsorption (two step process). The rate of As(III) oxidation with MnO2 is completed in two stages: rapid initially followed by a first order reaction. As(III) is oxidised to As(V) by the MnO2 with a release of approximately 1:1 molar Mn(II) into the solution. No significant pH effect on oxidation of As(III) was observed in the pH range 4 - 6. The rate showed a decreasing trend above pH 6. The removal of As(V) by adsorption on the MnO2 decreased significantly with increasing pH from 4 to 8. The adsorption capacity of the γ-MnO2 with particle size 90% passing 10 μm was determined to be 1.5 mg/g at pH 7. MnO2 was found to be more effective as an oxidant for As(III) in the two step process than in the one step process.展开更多
Fe2+ oxidation by Acidithiobacillus ferrooxidans(At.ferrooxidans) under different solid contents by adding inert Al2O3 powder was examined in rotating-drum and stirred-tank reactors.The results show that the bioact...Fe2+ oxidation by Acidithiobacillus ferrooxidans(At.ferrooxidans) under different solid contents by adding inert Al2O3 powder was examined in rotating-drum and stirred-tank reactors.The results show that the bioactivity of At.ferrooxidans in the stirred-tank is higher than that in the rotating-drum in the absence of Al2O3 powder,but the biooxidation rate of Fe2+ decreases markedly from 0.23 g/(L·h) to 0.025 g/(L·h) with increasing the content of Al2O3 powder from 0 to 50%(mass fraction) in the stirred-tank probably due to the deactivation of At.ferrooxidans resulting from the collision and friction of solid particles.The increase in Al2O3 content has a little adverse effect on the bioactivity of At.ferrooxidans in the rotating-drum due to different mixing mechanisms of the two reactors.The biooxidation rate of Fe2+ in the rotating-drum is higher than that in the stirred-tank at the same content of Al2O3 powder,especially at high solid content.The higher bioactivity of At.ferrooxidans can be maintained for allowing high solid content in the rotating-drum reactor,but its application potential still needs to be verified further by the sulfide bioleaching for the property differences of Al2O3 powder and sulfide minerals.展开更多
Picroside II,the major active component of picroside,has been shown to induce PC12 cell axonal growth and relieve free radical damage.In vivo experiments have demonstrated that picroside II can improve neurological fu...Picroside II,the major active component of picroside,has been shown to induce PC12 cell axonal growth and relieve free radical damage.In vivo experiments have demonstrated that picroside II can improve neurological function in rats with cerebral ischemia/reperfusion injuries.In the present in vivo study,enzyme-linked immunosorbent assay and immunohistochemistry revealed that picroside II increased superoxide dismutase content and reduced inducible nitric oxide synthase content in the ischemic hemisphere.The effects of picroside II were similar to those of salvianic acid A sodium,an active control drug.These results indicate that picroside II exerts a neuroprotective effect,possibly by downregulating inducible nitric oxide synthase expression,increasing superoxide dismutase activity,and inhibiting neuronal apoptosis.展开更多
Oxygenation constants and thermodynamic parameters DeltaH degrees and DeltaS degrees of cobalt (II) complexes with bis-(furaldehyde) Schiff bases (1, 2, 3, 4)were obtained by mearsuring saturated dioxygen uptake of th...Oxygenation constants and thermodynamic parameters DeltaH degrees and DeltaS degrees of cobalt (II) complexes with bis-(furaldehyde) Schiff bases (1, 2, 3, 4)were obtained by mearsuring saturated dioxygen uptake of these complexes in pyridine at different temperature. These complexes could activate molecular oxygen and were used as catalysts in cyclohexene oxidation. The influence of ligand structure on the dioxygen affinity and catalytic activity of the complexes were discussed.展开更多
Mixed iron-cobalt oxide (Co/Fe molar ratio = 1/5) are prepared using a simple co-precipitation procedure and studied for the catalytic oxidation of carbon monoxide. In particular, the effects of a range of preparati...Mixed iron-cobalt oxide (Co/Fe molar ratio = 1/5) are prepared using a simple co-precipitation procedure and studied for the catalytic oxidation of carbon monoxide. In particular, the effects of a range of preparation variables such as pH value when precipitation, aging temperature, precipitation agent type and aging time are investigated on the catalytic performance of synthesized Fe-Co oxides in CO oxidation reaction. In addition, the preparation factors were optimized by Taguchi design method. The optimized sample was characterized by XRD, N2 adsortion/desorption, TEM and TGA/DTA techniques. The results reveal that the optimized sample shows a mesoporous structure with a narrow pore size distribution centered in the range of 2-7 nm. The sample prepared under optimized conditions has high activity and stability toward removal of carbon monoxide at lower temperatures. It is shown that different preparation variables influence the catalytic performance of Fe-Co oxide in CO oxidation reaction.展开更多
Electrochemical water splitting into hydrogen and oxygen is a promising strategy for future renewable energy conversion devices.The oxygen evolution reaction(OER)is considered as the bottleneck reaction in an overall ...Electrochemical water splitting into hydrogen and oxygen is a promising strategy for future renewable energy conversion devices.The oxygen evolution reaction(OER)is considered as the bottleneck reaction in an overall water splitting system because it involves 4e- and 4H+ transfer processes.Currently,it is highly desirable to explore low-cost alternative catalysts for OER at ambient conditions.Herein,we report for the first time that nickel phosphide(Ni2P)nanosheets can be facilely grown on Fe foam(FF)as an efficient electrocatalyst for OER with excellent durability and catalytic activity under alkaline conditions.To reach a current density of 10 m A/cm2,the Ni2P-FF catalyst required a low overpotential of only 198 mV for OER.The catalyst’s high OER activity and durability were well maintained at a high current density.The required overpotentials were only 267 and 313 mV to achieve the current densities of 100 and 300 m A/cm2,respectively.The combination of low-cost Fe foam with Ni2P provides a promising low-cost catalyst for large-scale application of electrocatalytic water splitting.展开更多
A new crown ether appended Fe(Ⅲ) porphyrin complex was prepared by sulfuryl chloride appended benzo-15-crown-5 to the meso position of meso-5,10,15,20-tetra(4-hydrophenyl)porphyrin,and it was applied to catalytic...A new crown ether appended Fe(Ⅲ) porphyrin complex was prepared by sulfuryl chloride appended benzo-15-crown-5 to the meso position of meso-5,10,15,20-tetra(4-hydrophenyl)porphyrin,and it was applied to catalytic oxidation of cyclohexene with molecular oxygen without reductant,showing a remarkable catalytic activity(conversion is up to 94%) and selectivity for 2-cyclohexen-1-ol(73%).展开更多
基金The authors gratefully acknowledge financial support from the Ministry of Science and Technology of the People’s Republic of China(Grant Nos.2017YFC0210005 and 2016YFE0112200).
文摘Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex(Fe(III)-Ox).The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-Ox under solar irradiation.Although the photolysis mechanisms of Fe(III)-Ox have been investigated extensively,information about the oxidation of volatile organic compounds(VOC),specifically the potential for Secondary Organic Aerosol(SOA)formation in the Fe(III)-Ox system,is lacking.In this study,a ubiquitous VOC methacrolein(MACR)is chosen as a model VOC,and the oxidation of MACR with Fe(III)-Ox is investigated under typical atmospheric water conditions.The effects of oxalate concentration,Fe(III)concentration,MACR concentration,and pH on the oxidation of MACR are studied in detail.Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(III).The oxidation rate of MACR also accelerates with increasing concentration of oxalate.The effect of Fe(III)is found to be more complicated.The oxidation rate of MACR first increases and then decreases with increasing Fe(III)concentration.The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration.The production of ferrous and hydrogen peroxide,pH,and aqueous absorbance are monitored throughout the reaction process.The quenching experiments verify that·OH and O_(2)^(+)are both responsible for the oxidation of MACR.MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight,which contributes to the yield of SOA.These results suggest that Fe(III)-Ox plays an important role in atmospheric oxidation.
文摘Battery grade γ-MnO2 powder was investigated as an oxidant and an adsorbent in combination with Fe/Al coagulants for removal of arsenic from contaminated water. Simultaneous oxidation of As(III) and removal by coprecipitation/adsorption (one step process) was compared with pre-oxidation and subsequent removal by coprecipitation/adsorption (two step process). The rate of As(III) oxidation with MnO2 is completed in two stages: rapid initially followed by a first order reaction. As(III) is oxidised to As(V) by the MnO2 with a release of approximately 1:1 molar Mn(II) into the solution. No significant pH effect on oxidation of As(III) was observed in the pH range 4 - 6. The rate showed a decreasing trend above pH 6. The removal of As(V) by adsorption on the MnO2 decreased significantly with increasing pH from 4 to 8. The adsorption capacity of the γ-MnO2 with particle size 90% passing 10 μm was determined to be 1.5 mg/g at pH 7. MnO2 was found to be more effective as an oxidant for As(III) in the two step process than in the one step process.
基金Project(2010CB630904) supported by the National Basic Research Program of ChinaProject(5102030) supported by the Beijing Natural Science Foundation,China+1 种基金Projects(21076214,21006108) supported by the National Natural Science Foundation of ChinaProject supported by the Open Funding Project of the State Key Laboratory of Bioreactor Engineering,China
文摘Fe2+ oxidation by Acidithiobacillus ferrooxidans(At.ferrooxidans) under different solid contents by adding inert Al2O3 powder was examined in rotating-drum and stirred-tank reactors.The results show that the bioactivity of At.ferrooxidans in the stirred-tank is higher than that in the rotating-drum in the absence of Al2O3 powder,but the biooxidation rate of Fe2+ decreases markedly from 0.23 g/(L·h) to 0.025 g/(L·h) with increasing the content of Al2O3 powder from 0 to 50%(mass fraction) in the stirred-tank probably due to the deactivation of At.ferrooxidans resulting from the collision and friction of solid particles.The increase in Al2O3 content has a little adverse effect on the bioactivity of At.ferrooxidans in the rotating-drum due to different mixing mechanisms of the two reactors.The biooxidation rate of Fe2+ in the rotating-drum is higher than that in the stirred-tank at the same content of Al2O3 powder,especially at high solid content.The higher bioactivity of At.ferrooxidans can be maintained for allowing high solid content in the rotating-drum reactor,but its application potential still needs to be verified further by the sulfide bioleaching for the property differences of Al2O3 powder and sulfide minerals.
基金the National Natural Science Foundation of China, No. 30873391, 81041092
文摘Picroside II,the major active component of picroside,has been shown to induce PC12 cell axonal growth and relieve free radical damage.In vivo experiments have demonstrated that picroside II can improve neurological function in rats with cerebral ischemia/reperfusion injuries.In the present in vivo study,enzyme-linked immunosorbent assay and immunohistochemistry revealed that picroside II increased superoxide dismutase content and reduced inducible nitric oxide synthase content in the ischemic hemisphere.The effects of picroside II were similar to those of salvianic acid A sodium,an active control drug.These results indicate that picroside II exerts a neuroprotective effect,possibly by downregulating inducible nitric oxide synthase expression,increasing superoxide dismutase activity,and inhibiting neuronal apoptosis.
文摘Oxygenation constants and thermodynamic parameters DeltaH degrees and DeltaS degrees of cobalt (II) complexes with bis-(furaldehyde) Schiff bases (1, 2, 3, 4)were obtained by mearsuring saturated dioxygen uptake of these complexes in pyridine at different temperature. These complexes could activate molecular oxygen and were used as catalysts in cyclohexene oxidation. The influence of ligand structure on the dioxygen affinity and catalytic activity of the complexes were discussed.
基金supported by the University of Kashan (Grant No.158426/3)
文摘Mixed iron-cobalt oxide (Co/Fe molar ratio = 1/5) are prepared using a simple co-precipitation procedure and studied for the catalytic oxidation of carbon monoxide. In particular, the effects of a range of preparation variables such as pH value when precipitation, aging temperature, precipitation agent type and aging time are investigated on the catalytic performance of synthesized Fe-Co oxides in CO oxidation reaction. In addition, the preparation factors were optimized by Taguchi design method. The optimized sample was characterized by XRD, N2 adsortion/desorption, TEM and TGA/DTA techniques. The results reveal that the optimized sample shows a mesoporous structure with a narrow pore size distribution centered in the range of 2-7 nm. The sample prepared under optimized conditions has high activity and stability toward removal of carbon monoxide at lower temperatures. It is shown that different preparation variables influence the catalytic performance of Fe-Co oxide in CO oxidation reaction.
基金financially supported by the National Key Research and Development Program of China (2017YFA0402800)the National Natural Science Foundation of China (51772285)the National Synchrotron Radiation Laboratory at USTC.
文摘Electrochemical water splitting into hydrogen and oxygen is a promising strategy for future renewable energy conversion devices.The oxygen evolution reaction(OER)is considered as the bottleneck reaction in an overall water splitting system because it involves 4e- and 4H+ transfer processes.Currently,it is highly desirable to explore low-cost alternative catalysts for OER at ambient conditions.Herein,we report for the first time that nickel phosphide(Ni2P)nanosheets can be facilely grown on Fe foam(FF)as an efficient electrocatalyst for OER with excellent durability and catalytic activity under alkaline conditions.To reach a current density of 10 m A/cm2,the Ni2P-FF catalyst required a low overpotential of only 198 mV for OER.The catalyst’s high OER activity and durability were well maintained at a high current density.The required overpotentials were only 267 and 313 mV to achieve the current densities of 100 and 300 m A/cm2,respectively.The combination of low-cost Fe foam with Ni2P provides a promising low-cost catalyst for large-scale application of electrocatalytic water splitting.
基金the National Natural Science Foundation of China(No51063006)the Key Subject Foundation of Tianshui Normal University(NoTSA0818)for providing financial support for this project
文摘A new crown ether appended Fe(Ⅲ) porphyrin complex was prepared by sulfuryl chloride appended benzo-15-crown-5 to the meso position of meso-5,10,15,20-tetra(4-hydrophenyl)porphyrin,and it was applied to catalytic oxidation of cyclohexene with molecular oxygen without reductant,showing a remarkable catalytic activity(conversion is up to 94%) and selectivity for 2-cyclohexen-1-ol(73%).