Based on the hopping principle, a miniature gas fuel-powered hopper is designed and manufactured. According to thermodynamic analysis, the pressure-displacement curve in the combustion chamber after ignition is obtain...Based on the hopping principle, a miniature gas fuel-powered hopper is designed and manufactured. According to thermodynamic analysis, the pressure-displacement curve in the combustion chamber after ignition is obtained through iterative calculation, then the work on the cylinder done by high-pressure gas is calculated and the initial hopping velocity of the hopper is obtained. The wireless control system is developed to realize the tele-control of the hopper, including fuel injection and ignition. Experimental results agree well with analytical results. The hopper has a jumping ability of height 2.2 m and distance 3.5 m, and it is more than 14 times its dimension.展开更多
Intertidal macroalgae experience continual alternation of photosynthesis between aquatic state at high tide and aerial state at low tide. The comparative photosynthetic responses to inorganic carbon were investigated...Intertidal macroalgae experience continual alternation of photosynthesis between aquatic state at high tide and aerial state at low tide. The comparative photosynthetic responses to inorganic carbon were investigated in the common intertidal macroalga Ulva lactuca L. along the coast of Shantou between aquatic and aerial state. The inorganic carbon dissolved in seawater at present could fully (at 10 ℃ or 20 ℃) or nearly (at 30 ℃) saturate the aquatic photosynthesis of U. lactuca . However, the aerial photosynthesis was limited by current ambient atmospheric CO 2 level, and such a limitation was more severe at higher temperature (20-30 ℃) than at lower temperature (10 ℃). The carbon_saturated maximal photosynthesis of U. lactuca under aerial state was much greater than that under aquatic state at 10 ℃ and 20 ℃, while the maximal photosynthesis under both states was similar at 30 ℃. The aerial values of K m (CO 2) for photosynthesis were higher than the aquatic values. On the contrary, the values of apparent photosynthetic CO 2 conductance under aerial state were considerably lower than that under aquatic state. It was concluded that the increase of atmospheric CO 2 would enhance the primary productivity of U. lactuca through stimulating the photosynthesis under aerial state during low tide.展开更多
The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron ...The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron spectroscopy,H2 temperature-programmed reduction,O2 temperature-programmed desorption,and thermogravimetry-differential analysis.The catalytic performance of each of these materials during the selective oxidation of cyclohexane with oxygen in a solvent-free system was subsequently examined.It was found that the MnOx-500 catalyst,calcined at 500 °C,consisted of a Mn2O3 phase in addition to Mn5O8 and Mn3O4 phases and possessed a low surface area.Unlike MnOx-500,the MnOx-400 catalyst prepared at 400 °C was composed solely of Mn3O4 and Mn5O8 and had a higher surface area.The pronounced catalytic activity of this latter material for the oxidation of cyclohexene was determined to result from numerous factors,including a higher concentration of surface adsorbed oxygen,greater quantities of the surface Mn4+ ions that promote oxygen mobility and the extent of O2 adsorption and reducibility on the catalyst.The effects of various reaction conditions on the activity of the MnOx-400 during the oxidation of cyclohexane were also evaluated,such as the reaction temperature,reaction time,and initial oxygen pressure.Following a 4 h reaction at an initial O2 pressure of 0.5 MPa and 140 °C,an 8.0% cyclohexane conversion and 5.0% yield of cyclohexanol and cyclohexanone were achieved over the MnOx-400 catalyst.In contrast,employing MnOx-500 resulted in a 6.1% conversion of cyclohexane and 75% selectivity for cyclohexanol and cyclohexanone.After being recycled through 10 replicate uses,the catalytic activity of the MnOx-400 catalyst was unchanged,demonstrating its good stability.展开更多
Beijing experienced a long-lasting pollution episode in April 2012. Here, the authors characterize the sources and evolution processes of the pollution, with a focus on a haze and a dust episode that occurred during 1...Beijing experienced a long-lasting pollution episode in April 2012. Here, the authors characterize the sources and evolution processes of the pollution, with a focus on a haze and a dust episode that occurred during 15-30 April. All submicron aerosol species (PM1) showed substantial increases during the haze episode (HE), with nitrate being the largest, contributing on average 32.2% of the non-refractory PM;(NR-PM1) mass (maximum: -42.0%), which was different from other seasons. Secondary inorganic aerosol (SIA) species (55.1 ± 23.8 lag m-3; SIA = nitrate, ammonium, sulfate) played enhanced roles in the haze formation, accounting for 66.5% of the total NR-PM1 mass. In contrast to the HE, organics exhibited their highest levels (8.9 ± 5.4 lag m-3) among the NR-PM aerosol species during the dust episode, accounting for 64.0% on average. SIAs exhibited low concentration levels (4.6 ± 4.2 μg m-3) during the dust episode, contributing only 34.0% to the total NR-PM1 mass. This study suggests that air quality improvement strategies should be designed according to aerosol particle characteristics and formation mechanisms.展开更多
CO2 gasification of Fuijian high-metamorphous anthracite with black liquor (BL) and/or mixture of BL and calcium stuff (BL+Ca) as catalyst was studied by using a thermogravimetry under 750-950℃ at ambient pressu...CO2 gasification of Fuijian high-metamorphous anthracite with black liquor (BL) and/or mixture of BL and calcium stuff (BL+Ca) as catalyst was studied by using a thermogravimetry under 750-950℃ at ambient pressure. When the coal was impregnated with an appropriate quantity of Ca and BL mixture, the catalytic activity of CO2 gasification was enhanced obviously. With a loading of 8%Na-BL+2%Ca, the carbon conversion of three coal samples tested reaches up to 92.9%-99.3% at 950℃ within 30min. The continuous formation of alkali surface compounds such as ([-COM], [-CO2M]) and the presence of exchanged Ca, such as calcium phenolate and calcium carboxylates (COO)2Ca, contribute to the increase in catalytic efficiency, and using BL+Ca is more efficient than that adding BL only, The homogeneous model and shrinking-core model were applied to correlate the data of conversion with time and to estimate the reaction rate constants under different temperature. The corresponding reaction activation energy (Ea) and pre-exponential factor of three anthracites were estimated. It is found that Ea is in the range from 73.6 to 121.4kJ·mol^-1 in the case of BL+Ca, and 74.3 to 104.2kJ·mol^-1 when only BL was used as the catalyst, both of which are much less than that from 143.5 to 181.4kJ·mol^-1 if no catalyst used. It is clearly demonstrated that both of BL+Ca mixture and BL could be the source of cheap and effective catalyst for coal gasification.展开更多
The catalytic effects of single and mixed catalysts, i.e. single 3%Ca and 5%Na-BL(black liquor) catalysts and mixed 3%Ca+5%Na-BL catalyst, on carbon conversion, gasification reaction rate constant and activation en...The catalytic effects of single and mixed catalysts, i.e. single 3%Ca and 5%Na-BL(black liquor) catalysts and mixed 3%Ca+5%Na-BL catalyst, on carbon conversion, gasification reaction rate constant and activation energy, relative amount of harmful pollutant like sulphur containing gases have been investigated by thermogravimetry in steam gasification under temperature 750℃ to 950℃ at ambient pressure for three high-metarnorphous anthracites (Longyan, Fenghai and Youxia coals in Fujian Province). The mixed catalyst of 3%Ca+5%Na-BL increases greatly the carbon conversion and gasification rate constant by accelerating the gasification reaction C+H2O→CO+H2 due to presence of alkali surfacecompounds [COM], [CO2M] and exchanged calcium phenolate and calcium carboxylate (-COO)2. By adding CaCO3 into BL catalyst in gasification, in addition to improving the catalyst function and enhancing the carbon conversion, the effective desulphurization is also achieved, but the better operating temperature should be below 900℃. The homogenous and shrinking core models can be successfully employed to correlate the relations between the conversion and the gasification .time .and to estimate the reaction rate constant, The reaction acUvaUon energy and pre-exponential factor are estimated and the activation energy for mixed catalyst is in a range of 98.72-166.92 kJ·mol^-1, much less than 177.50-196.46 kJ·mol^-1 for non-catalytic steam gasification for three experimental coals.展开更多
77 K nitrogen adsorption was the most widely used technique for determining surface area and pore size distribution of coal. Brunauer–Emmett–Teller(BET) and Barrett–Joyner–Halenda(BJH) model are commonly used anal...77 K nitrogen adsorption was the most widely used technique for determining surface area and pore size distribution of coal. Brunauer–Emmett–Teller(BET) and Barrett–Joyner–Halenda(BJH) model are commonly used analytic methods for adsorption/desorption isotherm. A Chinese anthracite coal is tested in this study using an improved experimental method and adsorption isotherm analyzed by three adsorption mechanisms at different relative pressure stages. The result shows that the micropore filling adsorption predominates at the relative pressure stage from 6.8E 7 to 9E 3. Theoretically, BET and BJH model are not appropriate for analyzing coal samples which contain micropores. Two new analytic procedures for coal surface area and pore size distribution calculation are developed in this work. The results show that BET model underestimates surface area, and micropores smaller than 1.751 nm account for 35.5% of the total pore volume and 74.2% of the total surface area. The investigation of surface area and pore size distribution by incorporating the influence of micropore is significant for understanding adsorption mechanism of methane and carbon dioxide in coal.展开更多
The method of dangerous meteorological phenomenon detection using the data of coordinate measurement by receivers of global navigation satellite system (GLONASS) and global positioning system (GPS) is proposed. Th...The method of dangerous meteorological phenomenon detection using the data of coordinate measurement by receivers of global navigation satellite system (GLONASS) and global positioning system (GPS) is proposed. The possibility of thunderstorm courses and strong clouds detection on data of pseudo-distances and altitudes is shown theoretically and confirmed experimentally.展开更多
This paper introduces a new idea of controlling cavitation around a hydrofoil through a passive cavitation controller called artificial cavitation bubble generator (ACG). Cyclic processes, namely, growth and implosi...This paper introduces a new idea of controlling cavitation around a hydrofoil through a passive cavitation controller called artificial cavitation bubble generator (ACG). Cyclic processes, namely, growth and implosion of bubbles around an immersed body, are the main reasons for the destruction and erosion of the said body. This paper aims to create a condition in which the cavitation bubbles reach a steady-state situation and prevent the occurrence of the cyclic processes. For this purpose, the ACG is placed on the surface of an immersed body, in particular, the suction surface of a 2D hydrofoil. A simulation was performed with an implicit finite volume scheme based on a SIMPLE algorithm associated with the multiphase and cavitation model. The modified k-ε RNG turbulence model equipped with a modification of the turbulent viscosity was applied to overcome the turbulence closure problem. Numerical simulation of water flow over the hydrofoil equipped with the ACG shows that a low-pressure recirculation area is produced behind the ACG and artificially generates stationary cavitation bubbles. The location, shape, and size of this ACG are the crucial parameters in creating a proper control. Results show that the cavitation bubble is controlled well with a well-designed ACG.展开更多
A WRF-Chem model including a comprehensive gas-phase nitrogen chemistry module was used to simulate a severe dust event appearing in the eastern China on 19-25 March, 2002. The modeling result well reproduced PM10 con...A WRF-Chem model including a comprehensive gas-phase nitrogen chemistry module was used to simulate a severe dust event appearing in the eastern China on 19-25 March, 2002. The modeling result well reproduced PM10 concentrations in various distances from the dust sources and the transport pathway of the dust strom. The results showed that both the concentrations and the dry deposition fluxes of PM10 increased over the China seas during the dust event following the passage of a cold front system. The maximum fluxes of PM10 in the Yellow Sea and the East China Sea during the dust event were 5.5 and 8.4 times of those before the event, respectively. However, the temporal variations of the dry deposition fluxes of particulate inorganic nitrogen differed over the Yellow Sea from those over the East China Sea. Nitrate and ammonium in the whole northern China rapidly decreased because of the intrusion of dust-loaded air on 19 March. The dust plume arrived in the Yellow Sea on 20 March, decreasing the particulate inorganic nitrogen in mass concentration accordingly. The minimum dry deposition fluxes of nitrate and ammonium in the Yellow Sea were about 3/5 and 1/6 of those before the dust arrival, respectively. In contrast, when the dust plume crossed over the Yangtze Delta area, it became abundant in nitrate and ammonium and increased the concentrations and dry deposition fluxes of particulate inorganic nitrogen over the East China Sea, where the maximum dry deposition fluxes of nitrate and ammonium increased approximately by 4.1 and 2.6 times of those prior to the dust arrival.展开更多
Taking the saline lake bischofite and NH4Cl that was removed with the ammonia method and continuously followed by filtration as raw materials with a molar ratio of 1∶1 of MgCl2 to NH4Cl, ammonium carnallite was synth...Taking the saline lake bischofite and NH4Cl that was removed with the ammonia method and continuously followed by filtration as raw materials with a molar ratio of 1∶1 of MgCl2 to NH4Cl, ammonium carnallite was synthesized. And then the ammonium carnallite was dehydrated to some extent at 160℃ for 4 h. Ammonium carnallite reacted with ammonia at 240℃ for 150 min and the ammonation ammonium carnallite was produced. Finally, the ammonation ammonium carnallite was calcined at 750℃ into anhydrous magnesium chloride containing only 0.1%(mass fraction) of MgO. On the other hand, dehydrated ammonium carnallite was mixed with the solid ammonium chloride at mass ratio 1∶4 at high temperature and with the differential pressure of NH3 above 30.5kPa. The dehydrated ammonium carnallite of mixture was dehydrated at 410℃, and then calcined at 700℃ into anhydrous magnesium chloride with only 0.087%(mass fraction) of MgO. X-ray diffraction and electron microscopy analysis results prove that anhydrous magnesium chloride obtained by both methods hasn’t mixed phases, the particle is large and even has good dispersion, which is suitable for preparation of metal magnesium in the electrolysis.展开更多
The paper describes a method for monitoring CO2 leakage in geological carbon dioxide sequestration. A real time monitoring parameter, apparent leakage flux(ALF), is presented to monitor abnormal CO2 leakage, which can...The paper describes a method for monitoring CO2 leakage in geological carbon dioxide sequestration. A real time monitoring parameter, apparent leakage flux(ALF), is presented to monitor abnormal CO2 leakage, which can be calculated by atmospheric CO2 and O2 data. The computation shows that all ALF values are close to zero-line without the leakage. With a step change or linear perturbation of concentration to the initial CO2 concentration data with no leakage, ALF will deviate from background line. Perturbation tests prove that ALF method is sensitive to linear perturbation but insensitive to step change of concentration. An improved method is proposed based on real time analysis of surplus CO2 concentration in least square regression process, called apparent leakage flux from surplus analysis(ALFs), which is sensitive to both step perturbation and linear perturbations of concentration. ALF is capable of detecting concentration increase when the leakage occurs while ALFs is useful in all periods of leakage. Both ALF and ALFs are potential approaches to monitor CO2 leakage in geosequestration project.展开更多
Based on the recent research results on dry and wet deposition of nutrient elements and sulphate, we estimate the atmospheric flux of nutrient elements and sulphate to the southern Yellow Sea and the East China Sea in...Based on the recent research results on dry and wet deposition of nutrient elements and sulphate, we estimate the atmospheric flux of nutrient elements and sulphate to the southern Yellow Sea and the East China Sea in each season. The results suggest that the concentrations of nutrient elements and sulphate in aerosol and precipitation show an apparent seasonal cycle with the maximum values in winter and the minimum values in summer. Depositions of nitrate and sulphate are dominated by wet deposition, while the deposition for phosphate is mainly dry deposition. Moreover, compared with the riverine inputs, the atmospheric deposition may be the main source of dissolved inorganic nutrients in the southern Yellow Sea and the East China Sea.展开更多
Goethite is a metals-rich residue that occurs during zinc production. The feasibility of metal recovery from goethite has been demonstrated, but is not economically viable on an industrial scale. Therefore, goethite i...Goethite is a metals-rich residue that occurs during zinc production. The feasibility of metal recovery from goethite has been demonstrated, but is not economically viable on an industrial scale. Therefore, goethite is landfilled with considerable economic costs and environmental risks. The goal of this study is to evaluate the environmental performance of a new valorization strategy for goethite residues from zinc production, with the aims of: ① recovering the valuable zinc contained in the goethite and ② avoiding the landfilling of goethite by producing a clean byproduct. The presented goethite valoriza- tion strategy consists of a sequence of two processes: ① plasma fuming and ② inorganic polymerization of the fumed slag. Plasma fuming recovers the valuable metals by fuming the goethite. The metals-flee fumed slag undergoes a process of inorganic polymerization to form inorganic polymers, that can be used as a novel building material, as an alternative to ordinary Portland cement (OPC)-based concrete. Life- cycle assessment (LCA) is used to compare the environmental performance of the inorganic polymer with the environmental performances of equivalent OPC-based concrete. The LCA results show the tradeoff between the environmental burdens of the fuming process and inorganic polymerization versus the environmental benefits of metal recovery, OPC concrete substitution, and the avoidance of goethite land- filling. The goethite-based inorganic polymers production shows better performances in several environ- mental impact categories, thanks to the avoided landfilling of goethite. However, in other environmental impact categories, such as global warming, the goethite valorization is strongly affected by the high-energy requirements of the plasma-fuming process, which represent the environmental hotspots of the proposed goethite recycling scheme. The key elements toward the sustainability of goethite valorization have been identified, and include the use of a clean electric mix, more effective control of the fumed gas emissions, and a reduced use of fumed slag through increased efficiency of the inorganic polymerization process.展开更多
In a series of laboratory incubations using soils of two contrasting sitesfrom a temperate marsh on the Qinghai-Tibet Plateau, potential methane (CH_4) oxidation rates weremeasured to study the effects of inorganic N ...In a series of laboratory incubations using soils of two contrasting sitesfrom a temperate marsh on the Qinghai-Tibet Plateau, potential methane (CH_4) oxidation rates weremeasured to study the effects of inorganic N inputs on CH_4 oxidation. For adrained site, subsurfacepeat (5--15 cm) at an initial 20 mu L CH_4 L^(-1) showed a significantly different (P < 0.05) CH_4oxidation rate compared to other soil depths, with a maximal rate of 20.9 ng CH_4 gDW (dryweight)^(-1) h^(-1); the underlying mineral soil layers (15--30 and 30--50 cm) also had a strongCH_4 oxidation capacity at about an initial 2 000 mu L CH_4 L^(-1). With a waterlogged site, theCH_4 oxidation rate in an aerobic incubation was significantly greater (P < 0 05) in the surfacesoil layer (0--5 cm) compared to the 15--30 and 30--50 cm depths. There was generally no or a veryweak effect from addition of NO_3^- on CH_4 oxidation. In marked contrast, NH_4^+ salts, such as(NH_4)_2SO_4, NH_4Cl and NH_4NO_3, exhibited strong inhibitions, which varied as a function of theadded salts and the initial CH_4 level Increasing NH_4^+ usually resulted in greater inhibition andincreasing initial CH_4 concentrations resulted in less NH_4^+ inhibition on CH4 oxidation innatural high-altitude, low-latitude wetlands could be as important as has been reported foragricultural and forest soils. The NH_4^+ effects on the CH_4 oxidation rate need to be furtherinvestigated in a wide range of natural wetland soil types.展开更多
Pyridinic N is widely regarded as the active center while pyrrolic N has low‐activity in metal‐free N‐doped carbon for electrocatalytic CO_(2) reduction reaction(CO_(2)RR)to CO,but this viewpoint remains open to qu...Pyridinic N is widely regarded as the active center while pyrrolic N has low‐activity in metal‐free N‐doped carbon for electrocatalytic CO_(2) reduction reaction(CO_(2)RR)to CO,but this viewpoint remains open to question.In this study,through density functional theoretical calculations,we first illustrate that the intrinsic activity of pyrrolic N is high enough for effectively catalyzing CO_(2)RR,however,due to the interplay with the neighboring pyridinic N sites,the activity of pyrrolic N is dramatically suppressed.Then,experimentally,metal‐free N‐doped carbon spheres(NCS)electrocatalysts without significant pyridinic N content are prepared for CO_(2)RR.The pyrrolic N in NCS shows a direct‐positive correlation with the performance for CO_(2)RR,representing the active center with high activity.The optimum NCS could produce syngas with a wide range of CO/H_(2) ratio(0.09 to 12)in CO_(2)RR depending on the applied potential,meanwhile,the best selectivity of 71%for CO can be obtained.Intentionally adding a small amount of pyridinic N to the optimum NCS dramatically decreases the activity for CO_(2)RR,further verifying the suppressed activity of pyrrolic N sites by the neighboring pyridinic N sites.This work reveals the interaction between a variety of N species in N‐doped carbon,and the potential of pyrrolic N as the new type of active site for electrocatalysts,which can improve our understanding of the electrocatalysis mechanism and be helpful for the rational design of high‐efficient electrocatalysts.展开更多
Amorphous silicon films are prepared at lower temperature of 350 ℃ by new catalytic chemical vapor deposition method.In the method,material gases (SiH 4 and H 2) are decomposed by catalytic reaction at given temper...Amorphous silicon films are prepared at lower temperature of 350 ℃ by new catalytic chemical vapor deposition method.In the method,material gases (SiH 4 and H 2) are decomposed by catalytic reaction at given temperature,so a-Si films are deposited on substrates.It is found that a-Si films with high quality can be obtain,such as high photosensitivity of 10 6,low spin density of 2.5×10 16 cm -3 .展开更多
As a huge,intense,and elevated atmospheric heat source(AHS) approaching the mid-troposphere in spring and summer,the Tibetan Plateau(TP) thermal forcing is perceived as an important factor contributing to the formatio...As a huge,intense,and elevated atmospheric heat source(AHS) approaching the mid-troposphere in spring and summer,the Tibetan Plateau(TP) thermal forcing is perceived as an important factor contributing to the formation and variation of the Asian summer monsoon.Despite numerous studies devoted to determine the strength and change of the thermal forcing of the TP on the basis of various data sources and methods,uncertainties remain in quantitative estimation of the AHS and will persist for the following reasons:(1) Routine meteorological stations cover only limited regions and show remarkable spatial inhomogeneity with most distributed in the central and eastern plateau.Moreover,all of these stations are situated at an altitude below 5000 m.Thus,the large area above that elevation is not included in the data.(2) Direct observations on heat fluxes do not exist at most stations,and the sensible heat flux(SHF) is calculated by the bulk formula,in which the drag coefficient for heat is often treated as an empirical constant without considering atmospheric stability and thermal roughness length.(3) Radiation flux derived by satellite remote sensing shows a large discrepancy in the algorithm in data inversion and complex terrain.(4) In reanalysis data,besides the rare observational records employed for data assimilation,model bias in physical processes induces visible errors in producing the diabatic heating fields.展开更多
基金Supported by the National Natural Science Foundation of China(50605031)~~
文摘Based on the hopping principle, a miniature gas fuel-powered hopper is designed and manufactured. According to thermodynamic analysis, the pressure-displacement curve in the combustion chamber after ignition is obtained through iterative calculation, then the work on the cylinder done by high-pressure gas is calculated and the initial hopping velocity of the hopper is obtained. The wireless control system is developed to realize the tele-control of the hopper, including fuel injection and ignition. Experimental results agree well with analytical results. The hopper has a jumping ability of height 2.2 m and distance 3.5 m, and it is more than 14 times its dimension.
文摘Intertidal macroalgae experience continual alternation of photosynthesis between aquatic state at high tide and aerial state at low tide. The comparative photosynthetic responses to inorganic carbon were investigated in the common intertidal macroalga Ulva lactuca L. along the coast of Shantou between aquatic and aerial state. The inorganic carbon dissolved in seawater at present could fully (at 10 ℃ or 20 ℃) or nearly (at 30 ℃) saturate the aquatic photosynthesis of U. lactuca . However, the aerial photosynthesis was limited by current ambient atmospheric CO 2 level, and such a limitation was more severe at higher temperature (20-30 ℃) than at lower temperature (10 ℃). The carbon_saturated maximal photosynthesis of U. lactuca under aerial state was much greater than that under aquatic state at 10 ℃ and 20 ℃, while the maximal photosynthesis under both states was similar at 30 ℃. The aerial values of K m (CO 2) for photosynthesis were higher than the aquatic values. On the contrary, the values of apparent photosynthetic CO 2 conductance under aerial state were considerably lower than that under aquatic state. It was concluded that the increase of atmospheric CO 2 would enhance the primary productivity of U. lactuca through stimulating the photosynthesis under aerial state during low tide.
基金supported by the National Basic Research Program of China(973 Program,2010CB732300)the National Natural Science Foundation of China(21103048)~~
文摘The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron spectroscopy,H2 temperature-programmed reduction,O2 temperature-programmed desorption,and thermogravimetry-differential analysis.The catalytic performance of each of these materials during the selective oxidation of cyclohexane with oxygen in a solvent-free system was subsequently examined.It was found that the MnOx-500 catalyst,calcined at 500 °C,consisted of a Mn2O3 phase in addition to Mn5O8 and Mn3O4 phases and possessed a low surface area.Unlike MnOx-500,the MnOx-400 catalyst prepared at 400 °C was composed solely of Mn3O4 and Mn5O8 and had a higher surface area.The pronounced catalytic activity of this latter material for the oxidation of cyclohexene was determined to result from numerous factors,including a higher concentration of surface adsorbed oxygen,greater quantities of the surface Mn4+ ions that promote oxygen mobility and the extent of O2 adsorption and reducibility on the catalyst.The effects of various reaction conditions on the activity of the MnOx-400 during the oxidation of cyclohexane were also evaluated,such as the reaction temperature,reaction time,and initial oxygen pressure.Following a 4 h reaction at an initial O2 pressure of 0.5 MPa and 140 °C,an 8.0% cyclohexane conversion and 5.0% yield of cyclohexanol and cyclohexanone were achieved over the MnOx-400 catalyst.In contrast,employing MnOx-500 resulted in a 6.1% conversion of cyclohexane and 75% selectivity for cyclohexanol and cyclohexanone.After being recycled through 10 replicate uses,the catalytic activity of the MnOx-400 catalyst was unchanged,demonstrating its good stability.
基金supported by the National Key Basic Research Program of China[grant number 2014CB447900]the National Natural Science Foundation of China[grant number 41305115]+2 种基金the Strategic Priority Research Program(B)of the Chinese Academy of Sciences[grant number XDB05020501]the Project of High-resolution Earth Observation System[grant number 05-Y30B02-9001-13/15-7-WX02]Commonwealth Project in Ministry of Environmental Protection[grant number 201309011]
文摘Beijing experienced a long-lasting pollution episode in April 2012. Here, the authors characterize the sources and evolution processes of the pollution, with a focus on a haze and a dust episode that occurred during 15-30 April. All submicron aerosol species (PM1) showed substantial increases during the haze episode (HE), with nitrate being the largest, contributing on average 32.2% of the non-refractory PM;(NR-PM1) mass (maximum: -42.0%), which was different from other seasons. Secondary inorganic aerosol (SIA) species (55.1 ± 23.8 lag m-3; SIA = nitrate, ammonium, sulfate) played enhanced roles in the haze formation, accounting for 66.5% of the total NR-PM1 mass. In contrast to the HE, organics exhibited their highest levels (8.9 ± 5.4 lag m-3) among the NR-PM aerosol species during the dust episode, accounting for 64.0% on average. SIAs exhibited low concentration levels (4.6 ± 4.2 μg m-3) during the dust episode, contributing only 34.0% to the total NR-PM1 mass. This study suggests that air quality improvement strategies should be designed according to aerosol particle characteristics and formation mechanisms.
基金Supported by the National Natural Science Foundation of China (No.20376014) and Fujian Science and Technology Council Grant (HG99-01).
文摘CO2 gasification of Fuijian high-metamorphous anthracite with black liquor (BL) and/or mixture of BL and calcium stuff (BL+Ca) as catalyst was studied by using a thermogravimetry under 750-950℃ at ambient pressure. When the coal was impregnated with an appropriate quantity of Ca and BL mixture, the catalytic activity of CO2 gasification was enhanced obviously. With a loading of 8%Na-BL+2%Ca, the carbon conversion of three coal samples tested reaches up to 92.9%-99.3% at 950℃ within 30min. The continuous formation of alkali surface compounds such as ([-COM], [-CO2M]) and the presence of exchanged Ca, such as calcium phenolate and calcium carboxylates (COO)2Ca, contribute to the increase in catalytic efficiency, and using BL+Ca is more efficient than that adding BL only, The homogeneous model and shrinking-core model were applied to correlate the data of conversion with time and to estimate the reaction rate constants under different temperature. The corresponding reaction activation energy (Ea) and pre-exponential factor of three anthracites were estimated. It is found that Ea is in the range from 73.6 to 121.4kJ·mol^-1 in the case of BL+Ca, and 74.3 to 104.2kJ·mol^-1 when only BL was used as the catalyst, both of which are much less than that from 143.5 to 181.4kJ·mol^-1 if no catalyst used. It is clearly demonstrated that both of BL+Ca mixture and BL could be the source of cheap and effective catalyst for coal gasification.
基金Supported by the National Natural Science Foundation of China (20376014) and Fujian Science and Technology Council Grant (HG99-01 ).
文摘The catalytic effects of single and mixed catalysts, i.e. single 3%Ca and 5%Na-BL(black liquor) catalysts and mixed 3%Ca+5%Na-BL catalyst, on carbon conversion, gasification reaction rate constant and activation energy, relative amount of harmful pollutant like sulphur containing gases have been investigated by thermogravimetry in steam gasification under temperature 750℃ to 950℃ at ambient pressure for three high-metarnorphous anthracites (Longyan, Fenghai and Youxia coals in Fujian Province). The mixed catalyst of 3%Ca+5%Na-BL increases greatly the carbon conversion and gasification rate constant by accelerating the gasification reaction C+H2O→CO+H2 due to presence of alkali surfacecompounds [COM], [CO2M] and exchanged calcium phenolate and calcium carboxylate (-COO)2. By adding CaCO3 into BL catalyst in gasification, in addition to improving the catalyst function and enhancing the carbon conversion, the effective desulphurization is also achieved, but the better operating temperature should be below 900℃. The homogenous and shrinking core models can be successfully employed to correlate the relations between the conversion and the gasification .time .and to estimate the reaction rate constant, The reaction acUvaUon energy and pre-exponential factor are estimated and the activation energy for mixed catalyst is in a range of 98.72-166.92 kJ·mol^-1, much less than 177.50-196.46 kJ·mol^-1 for non-catalytic steam gasification for three experimental coals.
基金the China Scholarship Council and the Natural Science Foundation of China (No. 51174212)
文摘77 K nitrogen adsorption was the most widely used technique for determining surface area and pore size distribution of coal. Brunauer–Emmett–Teller(BET) and Barrett–Joyner–Halenda(BJH) model are commonly used analytic methods for adsorption/desorption isotherm. A Chinese anthracite coal is tested in this study using an improved experimental method and adsorption isotherm analyzed by three adsorption mechanisms at different relative pressure stages. The result shows that the micropore filling adsorption predominates at the relative pressure stage from 6.8E 7 to 9E 3. Theoretically, BET and BJH model are not appropriate for analyzing coal samples which contain micropores. Two new analytic procedures for coal surface area and pore size distribution calculation are developed in this work. The results show that BET model underestimates surface area, and micropores smaller than 1.751 nm account for 35.5% of the total pore volume and 74.2% of the total surface area. The investigation of surface area and pore size distribution by incorporating the influence of micropore is significant for understanding adsorption mechanism of methane and carbon dioxide in coal.
基金Task Complex Program National Academy of Sciences of Ukraine on Space Research for 2012-2016
文摘The method of dangerous meteorological phenomenon detection using the data of coordinate measurement by receivers of global navigation satellite system (GLONASS) and global positioning system (GPS) is proposed. The possibility of thunderstorm courses and strong clouds detection on data of pseudo-distances and altitudes is shown theoretically and confirmed experimentally.
文摘This paper introduces a new idea of controlling cavitation around a hydrofoil through a passive cavitation controller called artificial cavitation bubble generator (ACG). Cyclic processes, namely, growth and implosion of bubbles around an immersed body, are the main reasons for the destruction and erosion of the said body. This paper aims to create a condition in which the cavitation bubbles reach a steady-state situation and prevent the occurrence of the cyclic processes. For this purpose, the ACG is placed on the surface of an immersed body, in particular, the suction surface of a 2D hydrofoil. A simulation was performed with an implicit finite volume scheme based on a SIMPLE algorithm associated with the multiphase and cavitation model. The modified k-ε RNG turbulence model equipped with a modification of the turbulent viscosity was applied to overcome the turbulence closure problem. Numerical simulation of water flow over the hydrofoil equipped with the ACG shows that a low-pressure recirculation area is produced behind the ACG and artificially generates stationary cavitation bubbles. The location, shape, and size of this ACG are the crucial parameters in creating a proper control. Results show that the cavitation bubble is controlled well with a well-designed ACG.
基金supported by the National Science Foundation of China (No.40976063)International Cooperative Projects of MOST (No.2010DFA91350)
文摘A WRF-Chem model including a comprehensive gas-phase nitrogen chemistry module was used to simulate a severe dust event appearing in the eastern China on 19-25 March, 2002. The modeling result well reproduced PM10 concentrations in various distances from the dust sources and the transport pathway of the dust strom. The results showed that both the concentrations and the dry deposition fluxes of PM10 increased over the China seas during the dust event following the passage of a cold front system. The maximum fluxes of PM10 in the Yellow Sea and the East China Sea during the dust event were 5.5 and 8.4 times of those before the event, respectively. However, the temporal variations of the dry deposition fluxes of particulate inorganic nitrogen differed over the Yellow Sea from those over the East China Sea. Nitrate and ammonium in the whole northern China rapidly decreased because of the intrusion of dust-loaded air on 19 March. The dust plume arrived in the Yellow Sea on 20 March, decreasing the particulate inorganic nitrogen in mass concentration accordingly. The minimum dry deposition fluxes of nitrate and ammonium in the Yellow Sea were about 3/5 and 1/6 of those before the dust arrival, respectively. In contrast, when the dust plume crossed over the Yangtze Delta area, it became abundant in nitrate and ammonium and increased the concentrations and dry deposition fluxes of particulate inorganic nitrogen over the East China Sea, where the maximum dry deposition fluxes of nitrate and ammonium increased approximately by 4.1 and 2.6 times of those prior to the dust arrival.
基金Project(2000 G 101) supported by the Key Science and Technology Research Project of Qinghai Province
文摘Taking the saline lake bischofite and NH4Cl that was removed with the ammonia method and continuously followed by filtration as raw materials with a molar ratio of 1∶1 of MgCl2 to NH4Cl, ammonium carnallite was synthesized. And then the ammonium carnallite was dehydrated to some extent at 160℃ for 4 h. Ammonium carnallite reacted with ammonia at 240℃ for 150 min and the ammonation ammonium carnallite was produced. Finally, the ammonation ammonium carnallite was calcined at 750℃ into anhydrous magnesium chloride containing only 0.1%(mass fraction) of MgO. On the other hand, dehydrated ammonium carnallite was mixed with the solid ammonium chloride at mass ratio 1∶4 at high temperature and with the differential pressure of NH3 above 30.5kPa. The dehydrated ammonium carnallite of mixture was dehydrated at 410℃, and then calcined at 700℃ into anhydrous magnesium chloride with only 0.087%(mass fraction) of MgO. X-ray diffraction and electron microscopy analysis results prove that anhydrous magnesium chloride obtained by both methods hasn’t mixed phases, the particle is large and even has good dispersion, which is suitable for preparation of metal magnesium in the electrolysis.
基金Supported by the National Natural Science Foundation of China(51276141,20936004)
文摘The paper describes a method for monitoring CO2 leakage in geological carbon dioxide sequestration. A real time monitoring parameter, apparent leakage flux(ALF), is presented to monitor abnormal CO2 leakage, which can be calculated by atmospheric CO2 and O2 data. The computation shows that all ALF values are close to zero-line without the leakage. With a step change or linear perturbation of concentration to the initial CO2 concentration data with no leakage, ALF will deviate from background line. Perturbation tests prove that ALF method is sensitive to linear perturbation but insensitive to step change of concentration. An improved method is proposed based on real time analysis of surplus CO2 concentration in least square regression process, called apparent leakage flux from surplus analysis(ALFs), which is sensitive to both step perturbation and linear perturbations of concentration. ALF is capable of detecting concentration increase when the leakage occurs while ALFs is useful in all periods of leakage. Both ALF and ALFs are potential approaches to monitor CO2 leakage in geosequestration project.
基金This work is supported by the State"973"basic research program under contract(G19990437)the international cooperation program under contract(2001CB711004).
文摘Based on the recent research results on dry and wet deposition of nutrient elements and sulphate, we estimate the atmospheric flux of nutrient elements and sulphate to the southern Yellow Sea and the East China Sea in each season. The results suggest that the concentrations of nutrient elements and sulphate in aerosol and precipitation show an apparent seasonal cycle with the maximum values in winter and the minimum values in summer. Depositions of nitrate and sulphate are dominated by wet deposition, while the deposition for phosphate is mainly dry deposition. Moreover, compared with the riverine inputs, the atmospheric deposition may be the main source of dissolved inorganic nutrients in the southern Yellow Sea and the East China Sea.
文摘Goethite is a metals-rich residue that occurs during zinc production. The feasibility of metal recovery from goethite has been demonstrated, but is not economically viable on an industrial scale. Therefore, goethite is landfilled with considerable economic costs and environmental risks. The goal of this study is to evaluate the environmental performance of a new valorization strategy for goethite residues from zinc production, with the aims of: ① recovering the valuable zinc contained in the goethite and ② avoiding the landfilling of goethite by producing a clean byproduct. The presented goethite valoriza- tion strategy consists of a sequence of two processes: ① plasma fuming and ② inorganic polymerization of the fumed slag. Plasma fuming recovers the valuable metals by fuming the goethite. The metals-flee fumed slag undergoes a process of inorganic polymerization to form inorganic polymers, that can be used as a novel building material, as an alternative to ordinary Portland cement (OPC)-based concrete. Life- cycle assessment (LCA) is used to compare the environmental performance of the inorganic polymer with the environmental performances of equivalent OPC-based concrete. The LCA results show the tradeoff between the environmental burdens of the fuming process and inorganic polymerization versus the environmental benefits of metal recovery, OPC concrete substitution, and the avoidance of goethite land- filling. The goethite-based inorganic polymers production shows better performances in several environ- mental impact categories, thanks to the avoided landfilling of goethite. However, in other environmental impact categories, such as global warming, the goethite valorization is strongly affected by the high-energy requirements of the plasma-fuming process, which represent the environmental hotspots of the proposed goethite recycling scheme. The key elements toward the sustainability of goethite valorization have been identified, and include the use of a clean electric mix, more effective control of the fumed gas emissions, and a reduced use of fumed slag through increased efficiency of the inorganic polymerization process.
基金Project supported by the Knowledge Innovation Project in Resource and Environment Fields, Chinese Academy of Sciences (No. KZCX3-SW-128), the Open Foundation of the State Key Laboratory of Gas Geochemistry (SJJ-01-07), and the National Key Basic Research
文摘In a series of laboratory incubations using soils of two contrasting sitesfrom a temperate marsh on the Qinghai-Tibet Plateau, potential methane (CH_4) oxidation rates weremeasured to study the effects of inorganic N inputs on CH_4 oxidation. For adrained site, subsurfacepeat (5--15 cm) at an initial 20 mu L CH_4 L^(-1) showed a significantly different (P < 0.05) CH_4oxidation rate compared to other soil depths, with a maximal rate of 20.9 ng CH_4 gDW (dryweight)^(-1) h^(-1); the underlying mineral soil layers (15--30 and 30--50 cm) also had a strongCH_4 oxidation capacity at about an initial 2 000 mu L CH_4 L^(-1). With a waterlogged site, theCH_4 oxidation rate in an aerobic incubation was significantly greater (P < 0 05) in the surfacesoil layer (0--5 cm) compared to the 15--30 and 30--50 cm depths. There was generally no or a veryweak effect from addition of NO_3^- on CH_4 oxidation. In marked contrast, NH_4^+ salts, such as(NH_4)_2SO_4, NH_4Cl and NH_4NO_3, exhibited strong inhibitions, which varied as a function of theadded salts and the initial CH_4 level Increasing NH_4^+ usually resulted in greater inhibition andincreasing initial CH_4 concentrations resulted in less NH_4^+ inhibition on CH4 oxidation innatural high-altitude, low-latitude wetlands could be as important as has been reported foragricultural and forest soils. The NH_4^+ effects on the CH_4 oxidation rate need to be furtherinvestigated in a wide range of natural wetland soil types.
文摘Pyridinic N is widely regarded as the active center while pyrrolic N has low‐activity in metal‐free N‐doped carbon for electrocatalytic CO_(2) reduction reaction(CO_(2)RR)to CO,but this viewpoint remains open to question.In this study,through density functional theoretical calculations,we first illustrate that the intrinsic activity of pyrrolic N is high enough for effectively catalyzing CO_(2)RR,however,due to the interplay with the neighboring pyridinic N sites,the activity of pyrrolic N is dramatically suppressed.Then,experimentally,metal‐free N‐doped carbon spheres(NCS)electrocatalysts without significant pyridinic N content are prepared for CO_(2)RR.The pyrrolic N in NCS shows a direct‐positive correlation with the performance for CO_(2)RR,representing the active center with high activity.The optimum NCS could produce syngas with a wide range of CO/H_(2) ratio(0.09 to 12)in CO_(2)RR depending on the applied potential,meanwhile,the best selectivity of 71%for CO can be obtained.Intentionally adding a small amount of pyridinic N to the optimum NCS dramatically decreases the activity for CO_(2)RR,further verifying the suppressed activity of pyrrolic N sites by the neighboring pyridinic N sites.This work reveals the interaction between a variety of N species in N‐doped carbon,and the potential of pyrrolic N as the new type of active site for electrocatalysts,which can improve our understanding of the electrocatalysis mechanism and be helpful for the rational design of high‐efficient electrocatalysts.
文摘Amorphous silicon films are prepared at lower temperature of 350 ℃ by new catalytic chemical vapor deposition method.In the method,material gases (SiH 4 and H 2) are decomposed by catalytic reaction at given temperature,so a-Si films are deposited on substrates.It is found that a-Si films with high quality can be obtain,such as high photosensitivity of 10 6,low spin density of 2.5×10 16 cm -3 .
基金supported by the the National Natural Science Foundation of China (Grants 91337216 and 41175070)and the Open Project of the Key Laboratory of Meteorological Disaster of Ministry of Education (Grant KLME1309)
文摘As a huge,intense,and elevated atmospheric heat source(AHS) approaching the mid-troposphere in spring and summer,the Tibetan Plateau(TP) thermal forcing is perceived as an important factor contributing to the formation and variation of the Asian summer monsoon.Despite numerous studies devoted to determine the strength and change of the thermal forcing of the TP on the basis of various data sources and methods,uncertainties remain in quantitative estimation of the AHS and will persist for the following reasons:(1) Routine meteorological stations cover only limited regions and show remarkable spatial inhomogeneity with most distributed in the central and eastern plateau.Moreover,all of these stations are situated at an altitude below 5000 m.Thus,the large area above that elevation is not included in the data.(2) Direct observations on heat fluxes do not exist at most stations,and the sensible heat flux(SHF) is calculated by the bulk formula,in which the drag coefficient for heat is often treated as an empirical constant without considering atmospheric stability and thermal roughness length.(3) Radiation flux derived by satellite remote sensing shows a large discrepancy in the algorithm in data inversion and complex terrain.(4) In reanalysis data,besides the rare observational records employed for data assimilation,model bias in physical processes induces visible errors in producing the diabatic heating fields.