According to the configuration,mixed-conducting membranes are classified as symmetric membranes and asymmetric membranes consisting of a thin dense layer and a porous support.In this study,these two kinds of SrCo0.4Fe...According to the configuration,mixed-conducting membranes are classified as symmetric membranes and asymmetric membranes consisting of a thin dense layer and a porous support.In this study,these two kinds of SrCo0.4Fe0.5Zr0.1O3-δ oxide-based membranes were systematically compared in terms of oxygen permeability and chemical stability,and their differences were elucidated by means of the theoretical calculation.For the oxygen permeability,the asymmetric membrane was greater than the symmetric membrane due to the significant decrease of bulk diffusion resistance in the thin dense layer of the asymmetric membrane.In regard to the chemical stability,the increase of oxygen partial pressure on the asymmetric membrane surface at CH4 side produced the stable time of over 1032h in partial oxidation of methane at 1123K,while the symmetric membrane was only of 528h.This study demonstrated that the asymmetric membrane was a promising geometrical configuration for the practical application.展开更多
The thermal properties of a thermal barrier coating (TBC) system comprised of BaO-MgO-SiO_2 based glass-ceramic bond coating, 8% (mass fraction) yttria stabilized zirconia (8YSZ) top coating and nimonic alloy su...The thermal properties of a thermal barrier coating (TBC) system comprised of BaO-MgO-SiO_2 based glass-ceramic bond coating, 8% (mass fraction) yttria stabilized zirconia (8YSZ) top coating and nimonic alloy substrate were evaluated. The thermal diffusivity and thermal conductivity of the TBC coated substrate were lower than those of bare substrate and glass-ceramic coated substrate under identical conditions. The specific heat capacity, thermal diffusivity and thermal conductivity of the TBC coated substrate increase with the increase of the temperature. Further, it is observed that the thermal conductivity of the TBC system decreases with the increase in the top coating thickness.展开更多
Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-...Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-reduction method. The electrochemical stability of Tin O2n-1 was investigated and the results show almost no change in the redox region after oxidation for 20 h at 1.2 V(vs NHE) in 0.5 mol/L H2SO4 aqueous solution. The catalytic activity and stability of the Pt/Tin O2n-1 toward the oxygen reduction reaction(ORR) in 0.5 mol/L H2SO4 solution were investigated through the accelerated aging tests(AAT), and the morphology of the catalysts before and after the AAT was observed by transmission electron microscopy. At the potential of 0.55 V(vs SCE), the specific kinetic current density of the ORR on the Pt/Tin O2n-1 is about 1.5 times that of the Pt/C. The LSV curves for the Pt/C shift negatively obviously with the half-wave potential shifting about 0.02 V after 8000 cycles AAT, while no obvious change takes place for the LSV curves for the Pt/Tin O2n-1. The Pt particles supported on the carbon aggregate obviously, while the morphology of the Pt supported on Tin O2n-1 remains almost unchanged, which contributes to the electrochemical surface area loss of Pt/C being about 2times that of the Pt/Tin O2n-1. The superior catalytic stability of Pt/Tin O2n-1 toward the ORR could be attributed to the excellent stability of the Tin O2n-1 and the electronic interaction between the metals and the support.展开更多
The physicochemical features of phosphorus-modified ZSM-5 zeolites (SiO2/Al2O3 molar ratio is 25) were characterized by XRD(X-ray diffraction), BET(Brunauer, Emmett and Teller spcific surface area measurement), NH3-TP...The physicochemical features of phosphorus-modified ZSM-5 zeolites (SiO2/Al2O3 molar ratio is 25) were characterized by XRD(X-ray diffraction), BET(Brunauer, Emmett and Teller spcific surface area measurement), NH3-TPD(ammonia temperature-programmed desorption) and MASNMR(magic angle spinning nuclear magnetic resonance), and the performance on catalytic pyrolysis to produce ethylene was investigated with a light hydrocarbon fixed bed micro-reactor with n-octane as feed. The results show that the acid site density, acid intensity and hydrothermal stability of ZSM-5 zeolite were improved by phosphorus modification. When P2O5 content in ZSM-5 zeolite is higher than 2.5%, phosphorus modification can prevent ZSM-5 zeolite crystal structure transformation from orthorhombic to monoclinic. In addition, the dealumination of ZSM-5 zeolite framework was moderated by phosphorus modification under high temperature hydrothermal treatment. The results of n-octane pyrolysis on phosphorus-modified ZSM-5 zeolites show that ethylene yields of zeolites with different phosphorus content are almost the same under the same n-octane conversion. However, the modified zeolites with higher pyrolysis activity give lower yield of propene, butene and total olefin than lower pyrolysis activity under the same n-octane conversion.展开更多
Cu nanoparticles (CuNPs) have been synthesized through an easy route by chemical reduction at room temperature. The Cu^2+ ions were reduced and stabilized with sodium borohydride and polyvinylpyrrolidone, respectively...Cu nanoparticles (CuNPs) have been synthesized through an easy route by chemical reduction at room temperature. The Cu^2+ ions were reduced and stabilized with sodium borohydride and polyvinylpyrrolidone, respectively. The effect of the variation of the reducing agent/precursor-salt (RA/PS) ratio on the size and morphology of the CuNPs was evaluated. The synthesized material was studied by ultraviolet-visible (UV-Vis) spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The UV-Vis spectra showed a CuNPs plasmon peak at 569 nm and another peak belonging to Cu2O at 485 nm. XRD analysis showed the fcc-Cu phase with a small amount of fcc-Cu2O compound. SEM and TEM studies displayed that small semispherical CuNPs of approximately 7 nm were obtained at the RA/PS ratio of 2.6. The excess of polyvinylpyrrolidone stabilizer played an essential role in preventing CuNPs oxidation. On the other side, Cu2O polyhedral particles with larger sizes up to 150 nm were identified in the RA/PS ratio range of 2.0-1.84. In addition, Cu2O particles having star morphologies with quantum confinement at their tips were obtained at the RA/PS ratio of 1.66.展开更多
The chemical stability of cefixime was determined by high-performance liquid chromatography (HPLC) under different conditions, including factors such as pH, solvents, initial concentration, temperature and additives...The chemical stability of cefixime was determined by high-performance liquid chromatography (HPLC) under different conditions, including factors such as pH, solvents, initial concentration, temperature and additives. The degradation process follows the first-order kinetics. A pH-rate profile exhibits the U-shape and shows the maximum stability of cefixime at pH = 6. The stability in different pure solvents is ranked as acetone 〉 ethanol 〉 methanol 〉 water, while the degradation rate of cefixime exists a maximum at the ratio of 0.6 in water + methanol mixtures. In addition, the degradation rate increases with the temperature increasing and the activation energy of degradation was found to be 27.078 kJ. mol- 1 in acetone + water mixed solvents. The addition of different additives was proven to either inhibit or accelerate the degradation. The degradation products were analyzed using HPLC, LC-MS and infrared spectroscopy, and the possible degradation pathways in acid as well as alkaline environment were proposed to help us understand the degradation behavior of cefixime.展开更多
Chemical stability and reactivity of organic pollutants is dependent to their formation enthalpies. The main objective of this study is to provide simple straightforward strategy for prediction of the formation enthal...Chemical stability and reactivity of organic pollutants is dependent to their formation enthalpies. The main objective of this study is to provide simple straightforward strategy for prediction of the formation enthalpies of wide range organic pollutants only from their structural functional groups. Using such an extended dataset cornprising 1694 organic chemicals from 77 diverse material classes benefits the generalizability and reliability of the study. The new suggested collection of 12 functional groups and a simple linear regression lead to promising statis- tics of R2= 0.958, Q2 =0.956, and AEE= 57 kJ.mo1-1 for the whole dataset. Moreover, unknown experimental formation enthalpies for 27 organic pollutants are estimated by the presented approach. The resultant model needs no technical software/calculations, and thus can be easily applied by a non-specialist user.展开更多
High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,...High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,a widely-utilized“building block”in today’s chemical industry.Thus,it offers an intriguing and promising means to radically change the way of chemical manufacturing and achieve carbon neutrality using renewable energy sources,CO_(2),and water.Albeit with the great potential of HT-CO_(2)RR,this carbon utilization approach,unfortunately,has been suffering coke formation that is seriously detrimental to its energy efficiency and operating lifetime.In recent years,much effort has been added to understanding the mechanism of coke formation,managing reaction conditions to mitigate coke formation,and devising coke-formation-free electrode materials.These investigations have substantially advanced the HT-CO_(2)RR toward a practical industrial technology,but the resulting coke formation prevention strategies compromise activity and energy efficiency.Future research may target exploiting the control over both catalyst design and system design to gain selectivity,energy efficiency,and stability synchronously.Therefore,this perspective overviews the progress of research on coke formation in HT-CO_(2)RR,and elaborates on possible future directions that may accelerate its practical implementation at a large scale.展开更多
The synthesis and transport properties of the Li6La3BiSnO1212 solid electrolyte by a solid-state reaction were reported. The condition to synthesize the Li6La3BiSnO1212 is 785 °C for 36 h in air. The refined latt...The synthesis and transport properties of the Li6La3BiSnO1212 solid electrolyte by a solid-state reaction were reported. The condition to synthesize the Li6La3BiSnO1212 is 785 °C for 36 h in air. The refined lattice constant of Li6La3 BiSnO1212 is 13.007A. Qualitative phase analysis by X-ray powder diffraction patterns combined with the Rietveld method reveals garnet type compounds as major phases. The Li-ion conductivity of the prepared Li6La3BiSnO12 is 0.85×10^-4 S/cm at 22 °C, which is comparable with that of the Li5La3Bi2O12. The Li6La3BiSnO1212 compounds are chemically stable against Li CoO2 which is widely used as cathode material up to 700 °C but not against the Li Mn2O4 if the temperature is higher than 550 °C. The Li6La3 BiSnO1212 exhibits higher chemical stability than Li5La3Bi2O12, which is due to Sn substitution for Bi.展开更多
Nowadays, the electrochemical water treatments are very important methods used for the removal of organic and inorganic impurities from fresh, drinking water and wastewater. The method consists of carrying out the oxi...Nowadays, the electrochemical water treatments are very important methods used for the removal of organic and inorganic impurities from fresh, drinking water and wastewater. The method consists of carrying out the oxidation reaction at the anode where pollutants are transferred into non-toxic substances, by decomposing into simpler compounds or transferring into oxidation form. RuO2-based Dimensional Stable Anode (DSA) is a technologically good and important electrode for water treatment because of its unique characteristics such as high thermal and chemical stability, low resistivity and low overpotential. This paper reviews the methods for fabricating RuO2-based electrodes that can be used in electrochemical water treatment. Depending on the different fabrication routes, RuO2 electrodes will possess the different electro-catalytic property and stability.展开更多
Iron oxidation is a prevalent and important biogeochemical process in paddy soil,but little is known about whether and how microbially mediated iron oxidation is coupled with carbon assimilation,particularly under mic...Iron oxidation is a prevalent and important biogeochemical process in paddy soil,but little is known about whether and how microbially mediated iron oxidation is coupled with carbon assimilation,particularly under microaerobic conditions.Here,we investigated kinetics of CO_2 assimilation and Fe(Ⅱ)oxidation in an incubation experiment with paddy soil under suboxic conditions,and profiled the associated microbial community using DNA-stable isotope probing and 16S r RNA gene-based sequencing.The results showed that CO_2 assimilation and Fe(II)oxidation in the gradient tubes were predominantly mediated by the microbes enriched in the paddy soil,primarily Azospirillum and Magnetospirillum,as their relative abundances were higher in the^( 13)C heavy fractions compared to^( 12)C heavy fractions.This study provided direct evidence of chemoautotrophic microaerophiles linking iron oxidation and carbon assimilation at the oxic–anoxic interface in the paddy soil ecosystem.展开更多
基金Supported by the National Basic Research Program of China (2009CB623406), the National Natural Science Foundation of China (20636020), the National High Technology Research and Development Program of China (2006AA030204) and the Specialized Research Fund for the Doctoral Program of Higher Education of China (20060291003).
文摘According to the configuration,mixed-conducting membranes are classified as symmetric membranes and asymmetric membranes consisting of a thin dense layer and a porous support.In this study,these two kinds of SrCo0.4Fe0.5Zr0.1O3-δ oxide-based membranes were systematically compared in terms of oxygen permeability and chemical stability,and their differences were elucidated by means of the theoretical calculation.For the oxygen permeability,the asymmetric membrane was greater than the symmetric membrane due to the significant decrease of bulk diffusion resistance in the thin dense layer of the asymmetric membrane.In regard to the chemical stability,the increase of oxygen partial pressure on the asymmetric membrane surface at CH4 side produced the stable time of over 1032h in partial oxidation of methane at 1123K,while the symmetric membrane was only of 528h.This study demonstrated that the asymmetric membrane was a promising geometrical configuration for the practical application.
文摘The thermal properties of a thermal barrier coating (TBC) system comprised of BaO-MgO-SiO_2 based glass-ceramic bond coating, 8% (mass fraction) yttria stabilized zirconia (8YSZ) top coating and nimonic alloy substrate were evaluated. The thermal diffusivity and thermal conductivity of the TBC coated substrate were lower than those of bare substrate and glass-ceramic coated substrate under identical conditions. The specific heat capacity, thermal diffusivity and thermal conductivity of the TBC coated substrate increase with the increase of the temperature. Further, it is observed that the thermal conductivity of the TBC system decreases with the increase in the top coating thickness.
基金Project(21406273)supported by the National Natural Science Foundation of China
文摘Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-reduction method. The electrochemical stability of Tin O2n-1 was investigated and the results show almost no change in the redox region after oxidation for 20 h at 1.2 V(vs NHE) in 0.5 mol/L H2SO4 aqueous solution. The catalytic activity and stability of the Pt/Tin O2n-1 toward the oxygen reduction reaction(ORR) in 0.5 mol/L H2SO4 solution were investigated through the accelerated aging tests(AAT), and the morphology of the catalysts before and after the AAT was observed by transmission electron microscopy. At the potential of 0.55 V(vs SCE), the specific kinetic current density of the ORR on the Pt/Tin O2n-1 is about 1.5 times that of the Pt/C. The LSV curves for the Pt/C shift negatively obviously with the half-wave potential shifting about 0.02 V after 8000 cycles AAT, while no obvious change takes place for the LSV curves for the Pt/Tin O2n-1. The Pt particles supported on the carbon aggregate obviously, while the morphology of the Pt supported on Tin O2n-1 remains almost unchanged, which contributes to the electrochemical surface area loss of Pt/C being about 2times that of the Pt/Tin O2n-1. The superior catalytic stability of Pt/Tin O2n-1 toward the ORR could be attributed to the excellent stability of the Tin O2n-1 and the electronic interaction between the metals and the support.
文摘The physicochemical features of phosphorus-modified ZSM-5 zeolites (SiO2/Al2O3 molar ratio is 25) were characterized by XRD(X-ray diffraction), BET(Brunauer, Emmett and Teller spcific surface area measurement), NH3-TPD(ammonia temperature-programmed desorption) and MASNMR(magic angle spinning nuclear magnetic resonance), and the performance on catalytic pyrolysis to produce ethylene was investigated with a light hydrocarbon fixed bed micro-reactor with n-octane as feed. The results show that the acid site density, acid intensity and hydrothermal stability of ZSM-5 zeolite were improved by phosphorus modification. When P2O5 content in ZSM-5 zeolite is higher than 2.5%, phosphorus modification can prevent ZSM-5 zeolite crystal structure transformation from orthorhombic to monoclinic. In addition, the dealumination of ZSM-5 zeolite framework was moderated by phosphorus modification under high temperature hydrothermal treatment. The results of n-octane pyrolysis on phosphorus-modified ZSM-5 zeolites show that ethylene yields of zeolites with different phosphorus content are almost the same under the same n-octane conversion. However, the modified zeolites with higher pyrolysis activity give lower yield of propene, butene and total olefin than lower pyrolysis activity under the same n-octane conversion.
基金the National Council of Science and Technology (Conacyt) of Mexico for the financial support
文摘Cu nanoparticles (CuNPs) have been synthesized through an easy route by chemical reduction at room temperature. The Cu^2+ ions were reduced and stabilized with sodium borohydride and polyvinylpyrrolidone, respectively. The effect of the variation of the reducing agent/precursor-salt (RA/PS) ratio on the size and morphology of the CuNPs was evaluated. The synthesized material was studied by ultraviolet-visible (UV-Vis) spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The UV-Vis spectra showed a CuNPs plasmon peak at 569 nm and another peak belonging to Cu2O at 485 nm. XRD analysis showed the fcc-Cu phase with a small amount of fcc-Cu2O compound. SEM and TEM studies displayed that small semispherical CuNPs of approximately 7 nm were obtained at the RA/PS ratio of 2.6. The excess of polyvinylpyrrolidone stabilizer played an essential role in preventing CuNPs oxidation. On the other side, Cu2O polyhedral particles with larger sizes up to 150 nm were identified in the RA/PS ratio range of 2.0-1.84. In addition, Cu2O particles having star morphologies with quantum confinement at their tips were obtained at the RA/PS ratio of 1.66.
基金Supported by the National Natural Science Foundation of China(81361140344 and21376164)National High Technology Reseach and Development Program of China(863Program,2015AA021002)Major National Scientific Instrument Development Project(21527812)
文摘The chemical stability of cefixime was determined by high-performance liquid chromatography (HPLC) under different conditions, including factors such as pH, solvents, initial concentration, temperature and additives. The degradation process follows the first-order kinetics. A pH-rate profile exhibits the U-shape and shows the maximum stability of cefixime at pH = 6. The stability in different pure solvents is ranked as acetone 〉 ethanol 〉 methanol 〉 water, while the degradation rate of cefixime exists a maximum at the ratio of 0.6 in water + methanol mixtures. In addition, the degradation rate increases with the temperature increasing and the activation energy of degradation was found to be 27.078 kJ. mol- 1 in acetone + water mixed solvents. The addition of different additives was proven to either inhibit or accelerate the degradation. The degradation products were analyzed using HPLC, LC-MS and infrared spectroscopy, and the possible degradation pathways in acid as well as alkaline environment were proposed to help us understand the degradation behavior of cefixime.
基金Supported by the "Tehran Naftoon Arya Eng. Co." research committee of Iran
文摘Chemical stability and reactivity of organic pollutants is dependent to their formation enthalpies. The main objective of this study is to provide simple straightforward strategy for prediction of the formation enthalpies of wide range organic pollutants only from their structural functional groups. Using such an extended dataset cornprising 1694 organic chemicals from 77 diverse material classes benefits the generalizability and reliability of the study. The new suggested collection of 12 functional groups and a simple linear regression lead to promising statis- tics of R2= 0.958, Q2 =0.956, and AEE= 57 kJ.mo1-1 for the whole dataset. Moreover, unknown experimental formation enthalpies for 27 organic pollutants are estimated by the presented approach. The resultant model needs no technical software/calculations, and thus can be easily applied by a non-specialist user.
文摘High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,a widely-utilized“building block”in today’s chemical industry.Thus,it offers an intriguing and promising means to radically change the way of chemical manufacturing and achieve carbon neutrality using renewable energy sources,CO_(2),and water.Albeit with the great potential of HT-CO_(2)RR,this carbon utilization approach,unfortunately,has been suffering coke formation that is seriously detrimental to its energy efficiency and operating lifetime.In recent years,much effort has been added to understanding the mechanism of coke formation,managing reaction conditions to mitigate coke formation,and devising coke-formation-free electrode materials.These investigations have substantially advanced the HT-CO_(2)RR toward a practical industrial technology,but the resulting coke formation prevention strategies compromise activity and energy efficiency.Future research may target exploiting the control over both catalyst design and system design to gain selectivity,energy efficiency,and stability synchronously.Therefore,this perspective overviews the progress of research on coke formation in HT-CO_(2)RR,and elaborates on possible future directions that may accelerate its practical implementation at a large scale.
基金Project(51372278)supported by the National Natural Science Foundation of ChinaProject(2010RS4015)supported by the Natural Science Foundation of Hunan Province,China+1 种基金Project(2014ejing004)supported by the Hunan Intellectual Property Bureau,ChinaProject(CSUZC2014020)supported by the Open-End Fund for the Valuable and Precision Instruments of Central South University,China
文摘The synthesis and transport properties of the Li6La3BiSnO1212 solid electrolyte by a solid-state reaction were reported. The condition to synthesize the Li6La3BiSnO1212 is 785 °C for 36 h in air. The refined lattice constant of Li6La3 BiSnO1212 is 13.007A. Qualitative phase analysis by X-ray powder diffraction patterns combined with the Rietveld method reveals garnet type compounds as major phases. The Li-ion conductivity of the prepared Li6La3BiSnO12 is 0.85×10^-4 S/cm at 22 °C, which is comparable with that of the Li5La3Bi2O12. The Li6La3BiSnO1212 compounds are chemically stable against Li CoO2 which is widely used as cathode material up to 700 °C but not against the Li Mn2O4 if the temperature is higher than 550 °C. The Li6La3 BiSnO1212 exhibits higher chemical stability than Li5La3Bi2O12, which is due to Sn substitution for Bi.
文摘Nowadays, the electrochemical water treatments are very important methods used for the removal of organic and inorganic impurities from fresh, drinking water and wastewater. The method consists of carrying out the oxidation reaction at the anode where pollutants are transferred into non-toxic substances, by decomposing into simpler compounds or transferring into oxidation form. RuO2-based Dimensional Stable Anode (DSA) is a technologically good and important electrode for water treatment because of its unique characteristics such as high thermal and chemical stability, low resistivity and low overpotential. This paper reviews the methods for fabricating RuO2-based electrodes that can be used in electrochemical water treatment. Depending on the different fabrication routes, RuO2 electrodes will possess the different electro-catalytic property and stability.
基金funded by the National Natural Science Foundations of China(41420104007,41330857,and 41701295)Guangdong Natural Science Funds for Distinguished Young Scholar(2014A030306041)and Special Support Program(2016)
文摘Iron oxidation is a prevalent and important biogeochemical process in paddy soil,but little is known about whether and how microbially mediated iron oxidation is coupled with carbon assimilation,particularly under microaerobic conditions.Here,we investigated kinetics of CO_2 assimilation and Fe(Ⅱ)oxidation in an incubation experiment with paddy soil under suboxic conditions,and profiled the associated microbial community using DNA-stable isotope probing and 16S r RNA gene-based sequencing.The results showed that CO_2 assimilation and Fe(II)oxidation in the gradient tubes were predominantly mediated by the microbes enriched in the paddy soil,primarily Azospirillum and Magnetospirillum,as their relative abundances were higher in the^( 13)C heavy fractions compared to^( 12)C heavy fractions.This study provided direct evidence of chemoautotrophic microaerophiles linking iron oxidation and carbon assimilation at the oxic–anoxic interface in the paddy soil ecosystem.