It is crucial to understand the mechanism of low temperature CO oxidation reaction catalyzed by gold nanoparticles so as to find out the origin of the high catalytic reactivity and extend the indus‐trialization appli...It is crucial to understand the mechanism of low temperature CO oxidation reaction catalyzed by gold nanoparticles so as to find out the origin of the high catalytic reactivity and extend the indus‐trialization applications of nano gold catalysts. In this work, some theoretical works on CO adsorp‐tion, O2 adsorption, atomic oxygen adsorption, formation of surface gold oxide films, reaction mechanisms of CO oxidation involving O2 reaction with CO and O2 dissociation before reacting with CO on gold surfaces and Au/metal oxide were summarized, and the influences of coordination number, charge transfer and relativity of gold on CO oxidation reaction were briefly reviewed. It was found that CO reaction mechanism depended on the systems with or without oxide and the strong relativistic effects might play an important role in CO oxidation reaction on gold catalysts. In particular, the relativistic effects are related to the unique behaviors of CO adsorption, O adsorption, O2 activation on gold surfaces, effects of coordination number and the wide gap between the chem‐ical inertness of bulk gold and high catalytic activity of nano gold. The present work helps us to understand the CO oxidation reaction mechanism on gold catalysts and the influence of relativistic effects on gold catalysis.展开更多
By analyzing previous studies on activation energy of coal oxidation at low temperatures, a theoretical calculation model of apparent activation energy is established. Yield of CO is measured by using the characterist...By analyzing previous studies on activation energy of coal oxidation at low temperatures, a theoretical calculation model of apparent activation energy is established. Yield of CO is measured by using the characteristic detector of coal oxidation at 30-90 ℃. The impact of parameters, such as airflow and particle size, on activation energies is analyzed. Finally, agreement was obtained between activation energies and the dynamic oxygen absorbed in order to test the accuracy of the model. The results show that: 1) a positive exponential relation between concentration of CO and temperature in the process of the experiment is obtained: increases are almost identical and the initial CO is low; 2) the apparent activation energies increase gradually with the sizes of particle at the same airflow, but the gradients increase at a decreasing rate; 3) the apparent activation energies increase linearly with airflow. For the five coal particles, the differences among the energies are relatively high when the airflow was low, but the differences were low when the airflow was high; 4) the optimum sizes of particle, 0.125-0.25 ram, and the optimum volume of airflow, 100 mL/min, are determined from the model; 5) the apparent activation energies decrease with an increase in oxygen absorbed. A negative exponential relation between the two is obtained,展开更多
Based on the solubility in supercritical CO2,two strategies in which CO2 plays different roles are used to make quercetine and astaxanthin particles by supercritical fluid technologies.The experimental results showed ...Based on the solubility in supercritical CO2,two strategies in which CO2 plays different roles are used to make quercetine and astaxanthin particles by supercritical fluid technologies.The experimental results showed that micronized quercetine particles with mean particle size of 1.0-1.5 μm can be made via solution enhanced dispersion by supercritical fluids(SEDS) process,in which CO2 worked as turbulent anti-solvent;while for astaxanthin,micronized particles with mean particle size of 0.3-0.8 μm were also made successfully by rapid expansion supercritical solution(RESS) process.展开更多
A photocatalyst composed of TiO 2 nanotube arrays(TNTs) and octahedral Cu2 O nanoparticles was fabricated,and its performance in the photocatalytic reduction of CO2 under visible and simulated solar irradiation was ...A photocatalyst composed of TiO 2 nanotube arrays(TNTs) and octahedral Cu2 O nanoparticles was fabricated,and its performance in the photocatalytic reduction of CO2 under visible and simulated solar irradiation was studied. The average nanotube diameter and length was 100 nm and 5 μm,respectively. The different amount of octahedral Cu2 O modified TNTs were obtained by varying electrochemical deposition time. TNTs modified with an optimized amount of Cu2 O nanoparticles exhibited high efficiency in the photocatalysis,and the predominant hydrocarbon product was methane. The methane yield increased with increasing Cu2 O content of the catalyst up to a certain deposition time,and decreased with further increase in Cu2 O deposition time. Insufficient deposition time(5 min) resulted in a small amount of Cu2 O nanoparticles on the TNTs,leading to the disadvantage of harvesting light. However,excess deposition time(45 min) gave rise to entire TNT surface being most covered with Cu2 O nanoparticles with large sizes,inconvenient for the transport of photo-generated carriers. The highest methane yield under simulated solar and visible light irradiation was observed for the catalysts prepared at a Cu2 O deposition time of 15 and 30 min respectively. The morphology,crystallization,photoresponse and electrochemical properties of the catalyst were characterized to understand the mechanism of its high photocatalytic activity. The TNT structure provided abundant active sites for the adsorption of reactants,and promoted the transport of photogenerated carriers that improved charge separation. Modifying the TNTs with octahedral Cu2 O nanoparticles promoted light absorption,and prevented the hydrocarbon product from oxidation. These factors provided the Cu2O-modified TNT photocatalyst with high efficiency in the reduction of CO2,without requiring co-catalysts or sacrificial agents.展开更多
Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also...Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also strongly on the chemical nature of the iron oxide.In this study,Au NPs supported on iron oxide nanorods with different surface properties throughβ-FeOOH annealing,at varying temperatures,were synthesized,and applied in the CO oxidation.Detailed characterizations of the interactions between Au NPs and iron oxides were obtained by X-ray diffraction,transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy.The results indicate that the surface hydroxyl group on the Au/FeOOH catalyst,before calcination(Au/FeOOH-fresh),could facilitate the oxygen adsorption and dissociation on positively charged Au,thereby contributing to the low-temperature CO oxidation reactivity.After calcination at 200℃,under air exposure,the chemical state of the supported Au NP on varied iron oxides partly changed from metal cation to Au0,along with the disappearance of the surface OH species.Au/FeOOH with the highest Au0 content exhibits the highest activity in CO oxidation,among the as-synthesized catalysts.Furthermore,good durability in CO oxidation was achieved over the Au/FeOOH catalyst for 12 h without observable deactivation.In addition,the advanced identical-location TEM method was applied to the gas phase reaction to probe the structure evolution of the Au/iron oxide series of the catalysts and support structure.A Au NP size-dependent Ostwald ripening process mediated by the transport of Au(CO)x mobile species under certain reaction conditions is proposed,which offers a new insight into the validity of the structure-performance relationship.展开更多
The deposition onto an ordered mesoporous carbon(OMC)support of well dispersed PtM(M = Ru,Fe,Mo)alloy nanoparticles(NPs)were synthesized by a direct replication method using SBA-15 as the hard template,furfuryl ...The deposition onto an ordered mesoporous carbon(OMC)support of well dispersed PtM(M = Ru,Fe,Mo)alloy nanoparticles(NPs)were synthesized by a direct replication method using SBA-15 as the hard template,furfuryl alcohol and trimethylbeneze as the primary carbon sources,and metal acetylacetonate as the alloying metal precursor and secondary carbon source.The physicochemical properties of the PtM-OMC catalysts were characterized by N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,X-ray absorption near edge structure,and extended X-ray absorption fine structure.The alloy PtM NPs have an average size of 2-3 nm and were well dispersed in the pore channels of the OMC support.The second metal(M)in the PtM NPs was mostly in the reduced state,and formed a typical core(Pt)-shell(M)structure.Cyclic voltammetry measurements showed that these PtM-OMC electrodes had excellent electrocatalytic activities and tolerance to CO poisoning during the methanol oxidation reaction,which surpassed those of typical activated carbon-supported PtRu catalysts.In particular,the PtFe-OMC catalyst,which exhibited the best performance,can be a practical anodic electrocatalyst in direct methanol fuel cells due to its superior stability,excellent CO tolerance,and low production cost.展开更多
Magnetite is a kind of iron ore that is difficult to carburize.In order to improve the carburizing performance of magnetite pellet,pre-oxidation treatment was carried out,and the oxidation,reduction and carburization ...Magnetite is a kind of iron ore that is difficult to carburize.In order to improve the carburizing performance of magnetite pellet,pre-oxidation treatment was carried out,and the oxidation,reduction and carburization behaviors of magnetite pellet were investigated in this study.The magnetite pellet was oxidized in the air and carburized in CO-CO_(2)-H_(2) gas mixtures,the oxidation,reduction and carburization behaviors were demonstrated by detecting phase change,microstructure,carburizing index via thermogravimetry,X-ray diffraction(XRD),infrared carbon-sulfur analyzer,and scanning electron microscope(SEM).The results show that the dense magnetite particles inside pellet are oxidized to porous hematite particles,and the Fe_(3)O_(4) transforms to Fe_(2)O_(3) with high lattice defect concentration during the pre-oxidation process.Then the porous hematite particles and newly formed Fe_(2)O_(3) significantly promote the reduction efficiency.Porous metallic iron particles are produced in the reduction process.Finally,both high reduction efficiency and the porous structure of metallic iron particles dramatically enhance the carburization efficiency of pellet.High preoxidation temperature favors to the carburization of magnetite pellet.However,the carburized index decreases due to the recrystallization of iron oxide when the temperature extends to 1000℃.The optimum pre-oxidation temperature for magnetite pellet carburization is 900℃.展开更多
Porous medium has an obvious effect on the formation of carbon dioxide hydrate. In order to study the characteristics of CO2 hydrate formation in porous medium below the freezing point, the experiment of CO2 hydrate f...Porous medium has an obvious effect on the formation of carbon dioxide hydrate. In order to study the characteristics of CO2 hydrate formation in porous medium below the freezing point, the experiment of CO2 hydrate formation was conducted in a high-pressure 1.8-L cell in the presence of porous media with a particle size of 380 μm, 500 μm and 700 μm, respectively. The test results showed that the porous medium had an important influence on the process of CO2 hydrate formation below the freezing point. Compared with porous media with a particle size of 500 μm and 700 μm, respectively, the average hydrate formation rate and gas storage capacity of carbon dioxide hydrate in the porous medium with a particle size of 380 μm attained 0.016 14 mol/h and 65.094 L/L, respectively. The results also indicated that, within a certain range of particle sizes, the smaller the particle size of porous medium was, the larger the average hydrate formation rate and the gas storage capacity of CO2 hydrate during the process of hydrate formation would be.展开更多
The enhancement of chemical absorption of CO2 by K2CO3/H2O absorbents in the presence of activated carbon (AC) particles was investigated. The results show that the gas absorption rates can be enhanced significantly...The enhancement of chemical absorption of CO2 by K2CO3/H2O absorbents in the presence of activated carbon (AC) particles was investigated. The results show that the gas absorption rates can be enhanced significantly in the presence of AC particles, and the maximum enhancement factor 3.7 was observed at low stirring intensities. The enhancement factor increased rapidly with the solid loading during the initial period of absorption and then be- came mild gradually to a maximum value. Both the liquid-solid contact area and the probability of solid particles residing at the gas-liquid interface decreased with the increase of the particle size, leading to a negative effect on the enhancement of mass transfer. The influence of the particles on gas absorption decreased with the reaction rate. The stirring speed changed the interfacial coverage and mass transfer rate on the liquid side and consequently affected the mass transfer between the gas and liquid phases; the enhancement factor decreased with the stirring intensity. A heterogeneous two-zone model was proposed for predicting the enhancement factor and the calculated results agreed well with the experimental data.展开更多
High-temperature creep properties of sintered uranium dioxide pellets with two grain sizes (9.0 μm and 23.8μm) were studied. The results indicate that the creep rate becomes a little faster with the reduction of t...High-temperature creep properties of sintered uranium dioxide pellets with two grain sizes (9.0 μm and 23.8μm) were studied. The results indicate that the creep rate becomes a little faster with the reduction of the uranium dioxide grain size at the same temperature and the same load. At the same temperature, the logarithmic value of the steady creep rate vs stress has linear relation, and with increasing load, the steady creep rate of the sintered uranium dioxide pellet increases. Under the same load, the steady creep rate of the sintered uranium dioxide pellet increases with increasing temperature; and the creep rates of sintered uranium dioxide pellet with the grain size of 9.0 μm and 23.8 μm under 10 MPa are almost the same. The creep process is controlled both by Nabarro--Herring creep and Hamper-Dorn creep for uranium dioxide pellet with grain size of 9.0 μm, while Hamper---Dora creep is the dominantmechanism for uranium dioxide with grain size of 23.8 μm.展开更多
The denitrifying sulfide removal(DSR) process with bio-granules comprising both heterotrophic and autotrophic denitrifiers can simultaneously convert nitrate, sulfide and acetate species into di-nitrogen gas, elementa...The denitrifying sulfide removal(DSR) process with bio-granules comprising both heterotrophic and autotrophic denitrifiers can simultaneously convert nitrate, sulfide and acetate species into di-nitrogen gas, elemental sulfur and carbon dioxide, respectively, at high loading rates. This study has determined that the reaction rate of sulfide oxidized into sulfur could be enhanced in the presence of 1,2-naphthoquinone-4-sulphonate(NQS). The presence of NQS mitigated the inhibition effects of sulfide species on denitrification. Furthermore, the reaction rates of nitrate and acetate to nitrogen gas and CO_2, respectively, were also promoted in the presence of NQS, thereby enhancing the performance of DSR granules. The advantages and disadvantages of applying the NQS-DSR process are discussed.展开更多
The decomposition kinetics for formation of CO2 hydrates in 90 cm 3wet natural silica sands were studied systematically using the depressurization method at the temperatures ranging from 273.2 to 277.2 K and the press...The decomposition kinetics for formation of CO2 hydrates in 90 cm 3wet natural silica sands were studied systematically using the depressurization method at the temperatures ranging from 273.2 to 277.2 K and the pressures from 0.5 to 1.0 MPa.The effects of temperature,pressure,particle diameter,porosity,and salinity of formation water on the decomposition kinetics were investigated.The results show that the dissociation percentage increases as temperature increases or as the initial decomposition pressure decreases.An increase in porosity or a decrease in particle diameter of silica sands accelerates the decomposition.Increasing the salinity of the formation water gives rise to a faster decomposition.However,a combination of the present results with the observations in literature reveals that the effect of the coexisting ionic solute depends on its chemical structure.展开更多
A unique SiC whisker wheel was invented,in which the whiskers were aligned normally to the grinding wheel surface.In this paper,grindabilities of the SiC whisker wheel are investigated and compared with those of other...A unique SiC whisker wheel was invented,in which the whiskers were aligned normally to the grinding wheel surface.In this paper,grindabilities of the SiC whisker wheel are investigated and compared with those of other wheels of SiC grains,Al2O3 grains,as well as Al2O3 long and short fibres which were also aligned normally to the grinding wheel surface,respectively.The main research contents concern grinding characteristics of a directionally aligned SiC whisker wheel such as material-removal volume,wheel-wear rates,integrity of the ground surfaces,grinding ratios and grinding efficiency.Furthermore,grinding wheels of whiskers and fibres have a common disadvantage:they tend to load easily.The authors have proposed a simple method of loading-free grinding to overcome this propensity and investigate some related grinding characteristics under loading-free grinding conditions.展开更多
The effect of particle size on the recalcitrance of biochar against oxidation has been regarded as one of the most important factors influencing its stability and transportation in soils. Little is known about the pec...The effect of particle size on the recalcitrance of biochar against oxidation has been regarded as one of the most important factors influencing its stability and transportation in soils. Little is known about the peculiar stability of different particle sizes under chemical oxidation conditions. In this study, several sizes of biochar particles derived from beanpod were produced,and their stabilities were tested by using acid dichromate and hydrogen peroxide. We discovered that the 60-100 mesh size of particles produced at 400 and 500 ℃ showed the least carbon loss under the oxidation of both dichromate and hydrogen peroxide. In addition, this particle size also shows great stability at 600 and 700 ℃, but this stability was not observed below 300 °C for all temperature-dependent biochars. Medium-sized particles composed of exclusively heterogeneous components produced a biochar at temperatures over 400 ℃ with comparatively stronger chemical anti-oxidation characteristics. The chemical recalcitrance of biochar should be reevaluated based on particle size before soil application.展开更多
A magnetic bar carbon paste electrode (MBCPE) modified with Fe3O4 magnetic nanoparticles (Fe3O4NPs) and 2‐(3,4‐dihydroxyphenyl) benzothiazole (DPB) for the electrochemical determina‐tion of hydrazine was de...A magnetic bar carbon paste electrode (MBCPE) modified with Fe3O4 magnetic nanoparticles (Fe3O4NPs) and 2‐(3,4‐dihydroxyphenyl) benzothiazole (DPB) for the electrochemical determina‐tion of hydrazine was developed. The DPB was firstly self‐assembled on the Fe3O4NPs, and the re‐sulting Fe3O4NPs/DPB composite was then absorbed on the designed MBCPE. The MBCPE was used to attract the magnetic nanoparticles to the electrode surface. Owing to its high conductivity and large effective surface area, the novel electrode had a very large current response for the electrocat‐alytic oxidation of hydrazine. The modified electrode was characterized by voltammetry, scanning electron microscopy, electrochemical impedance spectroscopy, infrared spectroscopy, and UV‐visible spectroscopy. Voltammetric methods were used to study the electrochemical behaviour of hydrazine on MBCPE/Fe3O4NPs/DPB in phosphate buffer solution (pH = 7.0). The MBCPE/Fe3O4NPs/DPB, acting as an electrochemical sensor, exhibited very high electrocatalytic activity for the oxidation of hydrazine. The presence of DPB was found to reduce the oxidation potential of hydrazine and increase the catalytic current. The dependence of the electrocatalytic current on the hydrazine concentration exhibited two linear ranges, 0.1–0.4 μmol/L and 0.7–12.0 μmol/L, with a detection limit of 18.0 nmol/L. Additionally, the simultaneous determination of hydrazine and phe‐nol was investigated using the MBCPE/Fe3O4NPs/DPB electrode. Voltammetric experiments showed a linear range of 100–470 μmol/L and a detection limit of 24.3 μmol/L for phenol, and the proposed electrode was applied to the determination of hydrazine and phenol in water samples.展开更多
With the objective to investigate the structure-reactivity relationship of CuO/SnO2 and eventually design more applicable catalysts for soot combustion,catalysts with different CuO loadings have been prepared by impre...With the objective to investigate the structure-reactivity relationship of CuO/SnO2 and eventually design more applicable catalysts for soot combustion,catalysts with different CuO loadings have been prepared by impregnation method.By using X-ray diffraction and X-ray photoelectron spectroscopy extrapolation methods,it is disclosed that CuO disperses finely on the SnO2 support to form a monolayer with a capacity of 2.09 mmol 100 m^-2,which equals 4.8 wt%CuO loading.When the CuO loading is below the capacity,it is in a sub-monolayer state.However,when the loading is above the capacity,CuO micro-crystallites will be formed that coexist with the CuO monolayer.The soot combustion activity of the catalyst increases with the CuO loading until it reaches the monolayer dispersion capacity.A further increase in the CuO loading has no evident influence on the activity.Raman results have testified that with the addition of CuO onto the SnO2 support,a surface-active oxygen species can be formed,the amount of which also increases significantly with the increase in the CuO loading until it reaches the monolayer dispersion capacity.Increasing the CuO loading further has no evident impact on the amount of surface oxygen.Therefore,an apparent monolayer dispersion threshold effect is observed for soot combustion over CuO/SnO2 catalysts.It is concluded that the amount of surface-active oxygen sites is the major factor determining the activity of the catalyst.展开更多
In the Greater Casablanca, road transport is the second largest emissions source of gaseous pollutants and particles after the industry [ 1 ]. The emitters are mobile and include different categories of vehicles in ci...In the Greater Casablanca, road transport is the second largest emissions source of gaseous pollutants and particles after the industry [ 1 ]. The emitters are mobile and include different categories of vehicles in circulation, in the road network of the region [2]. Air emissions from road transport considered in this study are the exhaust emissions from combustion of fuel during vehicle movement. This is mainly SO2 (sulfur dioxide), NOx (nitrogen oxides), CO (carbon monoxide), CO2 (carbon dioxide), SP (suspended particulate) [3], VOC (volatile organic compounds), benzene, lead Pb and cadmium. These emissions depend mainly on the technology of the vehicle (type, fuel, engine size, and age), the vehicle speed, the engine temperature and ambient temperature [4].展开更多
We report on the ability to create complex 3D flower-like SiO2 in vitro via CaCO3 micropar- icles supported by polyethyleneimine mediated biosilicification under experimentally altered chemical influences. The morphol...We report on the ability to create complex 3D flower-like SiO2 in vitro via CaCO3 micropar- icles supported by polyethyleneimine mediated biosilicification under experimentally altered chemical influences. The morphology, structure, composition of the product have been inves- tigated with the X-ray photoelectron spectrum, scanning electron microscope, transmission electron microscope, and energy-dispersive spectroscopy. Tile overall morphologies could be controlled to shift from a characteristic network of flower-like silica sphere to a sheet-like structure by adjusting physical adsorption of different amount of polyethyleneimine onto the surface of the CaCO3 microparticles.展开更多
基金supported by the National Natural Science Foundation of China (21103165)
文摘It is crucial to understand the mechanism of low temperature CO oxidation reaction catalyzed by gold nanoparticles so as to find out the origin of the high catalytic reactivity and extend the indus‐trialization applications of nano gold catalysts. In this work, some theoretical works on CO adsorp‐tion, O2 adsorption, atomic oxygen adsorption, formation of surface gold oxide films, reaction mechanisms of CO oxidation involving O2 reaction with CO and O2 dissociation before reacting with CO on gold surfaces and Au/metal oxide were summarized, and the influences of coordination number, charge transfer and relativity of gold on CO oxidation reaction were briefly reviewed. It was found that CO reaction mechanism depended on the systems with or without oxide and the strong relativistic effects might play an important role in CO oxidation reaction on gold catalysts. In particular, the relativistic effects are related to the unique behaviors of CO adsorption, O adsorption, O2 activation on gold surfaces, effects of coordination number and the wide gap between the chem‐ical inertness of bulk gold and high catalytic activity of nano gold. The present work helps us to understand the CO oxidation reaction mechanism on gold catalysts and the influence of relativistic effects on gold catalysis.
基金Project 50474067 supported by National Natural Science Foundation of China
文摘By analyzing previous studies on activation energy of coal oxidation at low temperatures, a theoretical calculation model of apparent activation energy is established. Yield of CO is measured by using the characteristic detector of coal oxidation at 30-90 ℃. The impact of parameters, such as airflow and particle size, on activation energies is analyzed. Finally, agreement was obtained between activation energies and the dynamic oxygen absorbed in order to test the accuracy of the model. The results show that: 1) a positive exponential relation between concentration of CO and temperature in the process of the experiment is obtained: increases are almost identical and the initial CO is low; 2) the apparent activation energies increase gradually with the sizes of particle at the same airflow, but the gradients increase at a decreasing rate; 3) the apparent activation energies increase linearly with airflow. For the five coal particles, the differences among the energies are relatively high when the airflow was low, but the differences were low when the airflow was high; 4) the optimum sizes of particle, 0.125-0.25 ram, and the optimum volume of airflow, 100 mL/min, are determined from the model; 5) the apparent activation energies decrease with an increase in oxygen absorbed. A negative exponential relation between the two is obtained,
基金Supported partially by the China Ministry of Science and Technology for the China’s Agenda 21 Strategic Research (MOST,2008IM021900)the General Administration of Quality Supervision Inspection and Quarantine of the People’s Republic of China for the 4th Food Safety Research (AQSIQ 2008:ASPAQ0809)
文摘Based on the solubility in supercritical CO2,two strategies in which CO2 plays different roles are used to make quercetine and astaxanthin particles by supercritical fluid technologies.The experimental results showed that micronized quercetine particles with mean particle size of 1.0-1.5 μm can be made via solution enhanced dispersion by supercritical fluids(SEDS) process,in which CO2 worked as turbulent anti-solvent;while for astaxanthin,micronized particles with mean particle size of 0.3-0.8 μm were also made successfully by rapid expansion supercritical solution(RESS) process.
基金supported by the National Natural Science Foundation of China(2137704421573085)+5 种基金the Key Project of Natural Science Foundation of Hubei Province(2015CFA037)Wuhan Planning Project of Science and Technology(2014010101010023)Self-determined Research Funds of CCNU from the Colleges’Basic Research and Operation of MOE(CCNU15ZD007CCNU15KFY005)China Postdoctoral Science Foundation(2015M572187)Hubei Provincial Department of Education(D20152702)~~
文摘A photocatalyst composed of TiO 2 nanotube arrays(TNTs) and octahedral Cu2 O nanoparticles was fabricated,and its performance in the photocatalytic reduction of CO2 under visible and simulated solar irradiation was studied. The average nanotube diameter and length was 100 nm and 5 μm,respectively. The different amount of octahedral Cu2 O modified TNTs were obtained by varying electrochemical deposition time. TNTs modified with an optimized amount of Cu2 O nanoparticles exhibited high efficiency in the photocatalysis,and the predominant hydrocarbon product was methane. The methane yield increased with increasing Cu2 O content of the catalyst up to a certain deposition time,and decreased with further increase in Cu2 O deposition time. Insufficient deposition time(5 min) resulted in a small amount of Cu2 O nanoparticles on the TNTs,leading to the disadvantage of harvesting light. However,excess deposition time(45 min) gave rise to entire TNT surface being most covered with Cu2 O nanoparticles with large sizes,inconvenient for the transport of photo-generated carriers. The highest methane yield under simulated solar and visible light irradiation was observed for the catalysts prepared at a Cu2 O deposition time of 15 and 30 min respectively. The morphology,crystallization,photoresponse and electrochemical properties of the catalyst were characterized to understand the mechanism of its high photocatalytic activity. The TNT structure provided abundant active sites for the adsorption of reactants,and promoted the transport of photogenerated carriers that improved charge separation. Modifying the TNTs with octahedral Cu2 O nanoparticles promoted light absorption,and prevented the hydrocarbon product from oxidation. These factors provided the Cu2O-modified TNT photocatalyst with high efficiency in the reduction of CO2,without requiring co-catalysts or sacrificial agents.
基金supported by the National Natural Science Foundation of China(21773269,21761132025,91545119,21703262)the Youth Innovation Promotion Association CAS(2015152)+1 种基金the Joint Foundation of Liaoning Province Natural Science FoundationShenyang National Laboratory for Materials Science(20180510047)~~
文摘Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also strongly on the chemical nature of the iron oxide.In this study,Au NPs supported on iron oxide nanorods with different surface properties throughβ-FeOOH annealing,at varying temperatures,were synthesized,and applied in the CO oxidation.Detailed characterizations of the interactions between Au NPs and iron oxides were obtained by X-ray diffraction,transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy.The results indicate that the surface hydroxyl group on the Au/FeOOH catalyst,before calcination(Au/FeOOH-fresh),could facilitate the oxygen adsorption and dissociation on positively charged Au,thereby contributing to the low-temperature CO oxidation reactivity.After calcination at 200℃,under air exposure,the chemical state of the supported Au NP on varied iron oxides partly changed from metal cation to Au0,along with the disappearance of the surface OH species.Au/FeOOH with the highest Au0 content exhibits the highest activity in CO oxidation,among the as-synthesized catalysts.Furthermore,good durability in CO oxidation was achieved over the Au/FeOOH catalyst for 12 h without observable deactivation.In addition,the advanced identical-location TEM method was applied to the gas phase reaction to probe the structure evolution of the Au/iron oxide series of the catalysts and support structure.A Au NP size-dependent Ostwald ripening process mediated by the transport of Au(CO)x mobile species under certain reaction conditions is proposed,which offers a new insight into the validity of the structure-performance relationship.
基金supported by the Ministry of Science and Technology(NSC98-2113-M001-017-MY3,NSC101-2113-M001-020-MY3),Taiwan,China~~
文摘The deposition onto an ordered mesoporous carbon(OMC)support of well dispersed PtM(M = Ru,Fe,Mo)alloy nanoparticles(NPs)were synthesized by a direct replication method using SBA-15 as the hard template,furfuryl alcohol and trimethylbeneze as the primary carbon sources,and metal acetylacetonate as the alloying metal precursor and secondary carbon source.The physicochemical properties of the PtM-OMC catalysts were characterized by N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,X-ray absorption near edge structure,and extended X-ray absorption fine structure.The alloy PtM NPs have an average size of 2-3 nm and were well dispersed in the pore channels of the OMC support.The second metal(M)in the PtM NPs was mostly in the reduced state,and formed a typical core(Pt)-shell(M)structure.Cyclic voltammetry measurements showed that these PtM-OMC electrodes had excellent electrocatalytic activities and tolerance to CO poisoning during the methanol oxidation reaction,which surpassed those of typical activated carbon-supported PtRu catalysts.In particular,the PtFe-OMC catalyst,which exhibited the best performance,can be a practical anodic electrocatalyst in direct methanol fuel cells due to its superior stability,excellent CO tolerance,and low production cost.
基金Project(U1960104)supported by the National Natural Science Foundation of ChinaProject(LYU Ya-nan)supported by the Jiangsu Colleges and Universities Qing Lan Project,China。
文摘Magnetite is a kind of iron ore that is difficult to carburize.In order to improve the carburizing performance of magnetite pellet,pre-oxidation treatment was carried out,and the oxidation,reduction and carburization behaviors of magnetite pellet were investigated in this study.The magnetite pellet was oxidized in the air and carburized in CO-CO_(2)-H_(2) gas mixtures,the oxidation,reduction and carburization behaviors were demonstrated by detecting phase change,microstructure,carburizing index via thermogravimetry,X-ray diffraction(XRD),infrared carbon-sulfur analyzer,and scanning electron microscope(SEM).The results show that the dense magnetite particles inside pellet are oxidized to porous hematite particles,and the Fe_(3)O_(4) transforms to Fe_(2)O_(3) with high lattice defect concentration during the pre-oxidation process.Then the porous hematite particles and newly formed Fe_(2)O_(3) significantly promote the reduction efficiency.Porous metallic iron particles are produced in the reduction process.Finally,both high reduction efficiency and the porous structure of metallic iron particles dramatically enhance the carburization efficiency of pellet.High preoxidation temperature favors to the carburization of magnetite pellet.However,the carburized index decreases due to the recrystallization of iron oxide when the temperature extends to 1000℃.The optimum pre-oxidation temperature for magnetite pellet carburization is 900℃.
基金financially supported by the Natural Science Foundation of China (No. 51266005)the Science and Technology Research Key Project of the Ministry of Education (No. 1106ZBB007)+1 种基金the Hongliu Outstanding Talent Program of LUT (No. Q201101)the Open Fund of Natural Gas Hydrate Key Laboratory, Chinese Academy of Sciences (No. y007s3)
文摘Porous medium has an obvious effect on the formation of carbon dioxide hydrate. In order to study the characteristics of CO2 hydrate formation in porous medium below the freezing point, the experiment of CO2 hydrate formation was conducted in a high-pressure 1.8-L cell in the presence of porous media with a particle size of 380 μm, 500 μm and 700 μm, respectively. The test results showed that the porous medium had an important influence on the process of CO2 hydrate formation below the freezing point. Compared with porous media with a particle size of 500 μm and 700 μm, respectively, the average hydrate formation rate and gas storage capacity of carbon dioxide hydrate in the porous medium with a particle size of 380 μm attained 0.016 14 mol/h and 65.094 L/L, respectively. The results also indicated that, within a certain range of particle sizes, the smaller the particle size of porous medium was, the larger the average hydrate formation rate and the gas storage capacity of CO2 hydrate during the process of hydrate formation would be.
基金Supported by the National Natural Science Foundation of China (No.20176036).
文摘The enhancement of chemical absorption of CO2 by K2CO3/H2O absorbents in the presence of activated carbon (AC) particles was investigated. The results show that the gas absorption rates can be enhanced significantly in the presence of AC particles, and the maximum enhancement factor 3.7 was observed at low stirring intensities. The enhancement factor increased rapidly with the solid loading during the initial period of absorption and then be- came mild gradually to a maximum value. Both the liquid-solid contact area and the probability of solid particles residing at the gas-liquid interface decreased with the increase of the particle size, leading to a negative effect on the enhancement of mass transfer. The influence of the particles on gas absorption decreased with the reaction rate. The stirring speed changed the interfacial coverage and mass transfer rate on the liquid side and consequently affected the mass transfer between the gas and liquid phases; the enhancement factor decreased with the stirring intensity. A heterogeneous two-zone model was proposed for predicting the enhancement factor and the calculated results agreed well with the experimental data.
基金Project(50874126)supported by the National Natural Science Foundation of China
文摘High-temperature creep properties of sintered uranium dioxide pellets with two grain sizes (9.0 μm and 23.8μm) were studied. The results indicate that the creep rate becomes a little faster with the reduction of the uranium dioxide grain size at the same temperature and the same load. At the same temperature, the logarithmic value of the steady creep rate vs stress has linear relation, and with increasing load, the steady creep rate of the sintered uranium dioxide pellet increases. Under the same load, the steady creep rate of the sintered uranium dioxide pellet increases with increasing temperature; and the creep rates of sintered uranium dioxide pellet with the grain size of 9.0 μm and 23.8 μm under 10 MPa are almost the same. The creep process is controlled both by Nabarro--Herring creep and Hamper-Dorn creep for uranium dioxide pellet with grain size of 9.0 μm, while Hamper---Dora creep is the dominantmechanism for uranium dioxide with grain size of 23.8 μm.
基金supported bythe National Natural Science Foundation of China under Grant No. 21307160the Natural Science Foundation of Shandong Province under Grant No. ZR2013EEQ030
文摘The denitrifying sulfide removal(DSR) process with bio-granules comprising both heterotrophic and autotrophic denitrifiers can simultaneously convert nitrate, sulfide and acetate species into di-nitrogen gas, elemental sulfur and carbon dioxide, respectively, at high loading rates. This study has determined that the reaction rate of sulfide oxidized into sulfur could be enhanced in the presence of 1,2-naphthoquinone-4-sulphonate(NQS). The presence of NQS mitigated the inhibition effects of sulfide species on denitrification. Furthermore, the reaction rates of nitrate and acetate to nitrogen gas and CO_2, respectively, were also promoted in the presence of NQS, thereby enhancing the performance of DSR granules. The advantages and disadvantages of applying the NQS-DSR process are discussed.
基金Supported by the National Natural Science Foundation of China(40673043 20576073) the Program for New Century Excellent Talents in University from Ministry of Education of China(NCET-06-0088)
文摘The decomposition kinetics for formation of CO2 hydrates in 90 cm 3wet natural silica sands were studied systematically using the depressurization method at the temperatures ranging from 273.2 to 277.2 K and the pressures from 0.5 to 1.0 MPa.The effects of temperature,pressure,particle diameter,porosity,and salinity of formation water on the decomposition kinetics were investigated.The results show that the dissociation percentage increases as temperature increases or as the initial decomposition pressure decreases.An increase in porosity or a decrease in particle diameter of silica sands accelerates the decomposition.Increasing the salinity of the formation water gives rise to a faster decomposition.However,a combination of the present results with the observations in literature reveals that the effect of the coexisting ionic solute depends on its chemical structure.
文摘A unique SiC whisker wheel was invented,in which the whiskers were aligned normally to the grinding wheel surface.In this paper,grindabilities of the SiC whisker wheel are investigated and compared with those of other wheels of SiC grains,Al2O3 grains,as well as Al2O3 long and short fibres which were also aligned normally to the grinding wheel surface,respectively.The main research contents concern grinding characteristics of a directionally aligned SiC whisker wheel such as material-removal volume,wheel-wear rates,integrity of the ground surfaces,grinding ratios and grinding efficiency.Furthermore,grinding wheels of whiskers and fibres have a common disadvantage:they tend to load easily.The authors have proposed a simple method of loading-free grinding to overcome this propensity and investigate some related grinding characteristics under loading-free grinding conditions.
基金Supported by the Provincial Basic Research Program of Hebei Education Department(ZD2015110)the National Special Project on Key Technologies and Demonstration of Wetland Ecological Restoration in the Haihe River Basin(2014ZX07203008)the Fund of the University of Hebei Engineering(Grants 20120169)
文摘The effect of particle size on the recalcitrance of biochar against oxidation has been regarded as one of the most important factors influencing its stability and transportation in soils. Little is known about the peculiar stability of different particle sizes under chemical oxidation conditions. In this study, several sizes of biochar particles derived from beanpod were produced,and their stabilities were tested by using acid dichromate and hydrogen peroxide. We discovered that the 60-100 mesh size of particles produced at 400 and 500 ℃ showed the least carbon loss under the oxidation of both dichromate and hydrogen peroxide. In addition, this particle size also shows great stability at 600 and 700 ℃, but this stability was not observed below 300 °C for all temperature-dependent biochars. Medium-sized particles composed of exclusively heterogeneous components produced a biochar at temperatures over 400 ℃ with comparatively stronger chemical anti-oxidation characteristics. The chemical recalcitrance of biochar should be reevaluated based on particle size before soil application.
文摘A magnetic bar carbon paste electrode (MBCPE) modified with Fe3O4 magnetic nanoparticles (Fe3O4NPs) and 2‐(3,4‐dihydroxyphenyl) benzothiazole (DPB) for the electrochemical determina‐tion of hydrazine was developed. The DPB was firstly self‐assembled on the Fe3O4NPs, and the re‐sulting Fe3O4NPs/DPB composite was then absorbed on the designed MBCPE. The MBCPE was used to attract the magnetic nanoparticles to the electrode surface. Owing to its high conductivity and large effective surface area, the novel electrode had a very large current response for the electrocat‐alytic oxidation of hydrazine. The modified electrode was characterized by voltammetry, scanning electron microscopy, electrochemical impedance spectroscopy, infrared spectroscopy, and UV‐visible spectroscopy. Voltammetric methods were used to study the electrochemical behaviour of hydrazine on MBCPE/Fe3O4NPs/DPB in phosphate buffer solution (pH = 7.0). The MBCPE/Fe3O4NPs/DPB, acting as an electrochemical sensor, exhibited very high electrocatalytic activity for the oxidation of hydrazine. The presence of DPB was found to reduce the oxidation potential of hydrazine and increase the catalytic current. The dependence of the electrocatalytic current on the hydrazine concentration exhibited two linear ranges, 0.1–0.4 μmol/L and 0.7–12.0 μmol/L, with a detection limit of 18.0 nmol/L. Additionally, the simultaneous determination of hydrazine and phe‐nol was investigated using the MBCPE/Fe3O4NPs/DPB electrode. Voltammetric experiments showed a linear range of 100–470 μmol/L and a detection limit of 24.3 μmol/L for phenol, and the proposed electrode was applied to the determination of hydrazine and phenol in water samples.
基金supported by the National Natural Science Foundation of China(21567016,21666020)the Natural Science Foundation of Jiangxi Province(20181ACB20005,20171BAB213013,20181BCD40004,20181BAB203017)+2 种基金the Innovation Fund Designated for Graduate Students of Jiangxi Province(YC2018-B015)the Education Department Foundation of Jiangxi Province(KJLD14005)the Opening Fund of Key Laboratory of Process Analysis and Control of Sichuan Universities(2017002)~~
文摘With the objective to investigate the structure-reactivity relationship of CuO/SnO2 and eventually design more applicable catalysts for soot combustion,catalysts with different CuO loadings have been prepared by impregnation method.By using X-ray diffraction and X-ray photoelectron spectroscopy extrapolation methods,it is disclosed that CuO disperses finely on the SnO2 support to form a monolayer with a capacity of 2.09 mmol 100 m^-2,which equals 4.8 wt%CuO loading.When the CuO loading is below the capacity,it is in a sub-monolayer state.However,when the loading is above the capacity,CuO micro-crystallites will be formed that coexist with the CuO monolayer.The soot combustion activity of the catalyst increases with the CuO loading until it reaches the monolayer dispersion capacity.A further increase in the CuO loading has no evident influence on the activity.Raman results have testified that with the addition of CuO onto the SnO2 support,a surface-active oxygen species can be formed,the amount of which also increases significantly with the increase in the CuO loading until it reaches the monolayer dispersion capacity.Increasing the CuO loading further has no evident impact on the amount of surface oxygen.Therefore,an apparent monolayer dispersion threshold effect is observed for soot combustion over CuO/SnO2 catalysts.It is concluded that the amount of surface-active oxygen sites is the major factor determining the activity of the catalyst.
文摘In the Greater Casablanca, road transport is the second largest emissions source of gaseous pollutants and particles after the industry [ 1 ]. The emitters are mobile and include different categories of vehicles in circulation, in the road network of the region [2]. Air emissions from road transport considered in this study are the exhaust emissions from combustion of fuel during vehicle movement. This is mainly SO2 (sulfur dioxide), NOx (nitrogen oxides), CO (carbon monoxide), CO2 (carbon dioxide), SP (suspended particulate) [3], VOC (volatile organic compounds), benzene, lead Pb and cadmium. These emissions depend mainly on the technology of the vehicle (type, fuel, engine size, and age), the vehicle speed, the engine temperature and ambient temperature [4].
文摘We report on the ability to create complex 3D flower-like SiO2 in vitro via CaCO3 micropar- icles supported by polyethyleneimine mediated biosilicification under experimentally altered chemical influences. The morphology, structure, composition of the product have been inves- tigated with the X-ray photoelectron spectrum, scanning electron microscope, transmission electron microscope, and energy-dispersive spectroscopy. Tile overall morphologies could be controlled to shift from a characteristic network of flower-like silica sphere to a sheet-like structure by adjusting physical adsorption of different amount of polyethyleneimine onto the surface of the CaCO3 microparticles.