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1.
Aggregate structure of covalently functionalized chiral specific semiconducting single-walled carbon nanotubes (SWNTs) was systematically studied employing static light scattering (SLS). Fractal dimensions (Df) of two specific chirality SWNTs—SG65 and SG76 with (6, 5) and (7, 6) chiral enrichments—were measured under four biological exposure media conditions, namely: Dulbecco’s Modified Eagle Medium (DMEM), Minimum Essential Medium (MEM), Roswell Park Memorial Institute (RPMI) 1640 medium, and 0.9% saline solution. The SWNTs exhibited chiral dependence on Df with SG65 showing more fractal or loosely bound aggregate structures, i.e., lower Df values (range of 2.24 ± 0.03 to 2.64 ± 0.05), compared to the SG76 sample (range of 2.58 ± 0.13 to 2.90 ± 0.08). All the Df values reported are highly reproducible, measured from multiple SLS runs and estimated with ‘random block-effects’ statistical analysis that yielded all p values to be <0.001. The key mechanism for such difference in Df between the SWNT samples was identified as the difference in van der Waals (VDW) interaction energies of these samples, where higher VDW of SG76 resulted in tighter packing density. Effect of medium type showed lower sensitivity; however, presence of di-valent cations (Ca2+) in DMEM and MEM media resulted in relatively loose or more fractal aggregates. Moreover, presence of fetal bovine serum (FBS) and bovine serum albumin (BSA), used to mimic the in vitro cell culture condition, reduced the Df values, i.e., created more fractal structures. Steric hindrance to aggregation was identified as the key mechanism for creating the fractal structures. Also, increase in FBS concentration from 1% to 10% resulted in increasingly lower Df values.  相似文献   

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3.
Different aspects of visibility degradation problems in Brisbane were investigated through concurrent visibility monitoring and aerosol sampling programs carried out in 1995. The relationship between the light extinction coefficients and aerosol mass/composition was derived by using multiple linear regression techniques. The visibility properties at different sites in Brisbane were found to be correlated with each other on a daily basis, but not correlated with each other hour by hour. The cause of scattering of light by moisture (bsw) was due to sulphate particles which shift to a larger size under high-humidity conditions. The scattering of light by particulate matter (bsp) was found to be highly correlated with the mass of fine aerosols, in particular the mass of fine soot, sulphate and non-soil K. For the period studied, on average, the total light extinction coefficient (bext) at five sites in Brisbane was 0.65×10−4 m−1, considerably smaller than those values found in other Australian and overseas cities. On average, the major component of bext is bsp (49% of bext), followed by bap (the absorption of light, mainly by fine soot particles, 28%), bsg (Rayleigh scattering, 20%) and bsw (3%). The absorption of light by NO2 (bag) is expected to contribute less than 5% of bext. On average, the percentage contribution of the visibility degrading species to bext (excluding bag) were: soot (53%), sulphate (21%), Rayleigh scattering (20%), non-soil K (2%) and humidity (3%). In terms of visibility degrading sources, motor vehicles (including soot and the secondary products) are expected to contribute more than half of the bext (excluding bag) in Brisbane on average, followed by secondary sulphates (17%) and biomass burning (10%).  相似文献   

4.
A wide range of environmental particulate matter (PM) both indoor and outdoor and consisting of natural and anthropogenic PM was collected by high volume air filters, electrostatic precipitation, and thermophoretic precipitation directly onto transmission electron microscope (TEM) coated grid platforms. These collected PM have been systematically characterized by TEM, energy-dispersive X-ray spectrometry (EDS) and scanning electron microscopy (SEM). In the El Paso, TX, USA/Juarez, Mexico metroplex 93% of outdoor PM1 is crystalline while 40% of PM1 is carbonaceous soot (including multiwall carbon nanotubes (MWCNTs) and multiconcentric fullerenes) PM. Multiply-replicated cytotoxicity (in vitro) assays utilizing a human epithelial (lung model) cell line (A549) consistently demonstrated varying degrees of cell death for essentially all PM which was characterized as aggregates of nanoparticulates or primary nanoparticles. Cytokine release was detected for Fe2O3, chrysotile asbestos, BC, and MWCNT PM while reactive oxygen species (ROS) production has been detected for Fe2O3, asbestos, BC, and MWCNT aggregate PM as well as natural gas combustion PM.Nanoparticulate materials in the indoor and outdoor environments appear to be variously cytotoxic, especially carbonaceous nano-PM such as multiwall carbon nanotubes, black carbon, and soot nano-PM produced by natural gas combustion.  相似文献   

5.
In developed nations people spend about 90% of their time indoors. The relationship between indoor and outdoor air pollution levels is important for the understanding of the health effects of outdoor air pollution. Although other studies describe both the outdoor and indoor atmospheric environment, few excluded a priori major indoor sources, measured the air exchange rate, included more than one micro-environment and included the presence of human activity. PM2.5, soot, NO2 and the air exchange rate were measured during winter and summer indoors and outdoors at 18 homes (mostly apartments) of 18 children (6–11-years-old) and also at the six schools and 10 pre-schools that the children attended. The three types of indoor environments were free of environmental tobacco smoke and gas appliances, as the aim was to asses to what extent PM2.5, soot and NO2 infiltrate from outdoors to indoors. The median indoor and outdoor PM2.5 levels were 8.4 μg m?3 and 9.3 μg m?3, respectively. The median indoor levels for soot and NO2 were 0.66 m?1 × 10?5 and 10.0 μg m?3, respectively. The respective outdoor levels were 0.96 m?1 × 10?5 and 12.4 μg m?3. The median indoor/outdoor (I/O) ratios were 0.93, 0.76 and 0.92 for PM2.5, soot and NO2, respectively. Their infiltration factors were influenced by the micro-environment, ventilation type and air exchange rate, with aggregated values of 0.25, 0.55 and 0.64, respectively. Indoor and outdoor NO2 levels were strongly associated (R2 = 0.71), followed by soot (R2 = 0.50) and PM2.5 (R2 = 0.16). In Stockholm, the three major indoor environments occupied by children offer little protection against combustion-related particles and gases in the outdoor air. Outdoor PM2.5 seems to infiltrate less, but indoor sources compensate.  相似文献   

6.

The influences of relative humidity (RH) on the heterogeneous reaction of NO2 with soot were investigated by a coated wall flow tube reactor at ambient pressure. The initial uptake coefficient (γ initial) of NO2 showed a significant decrease with increasing RH from 7 to 70%. The γ initial on “fuel-rich” and “fuel-lean” soot at RH = 7% was (2.59 ± 0.20) × 10?5 and (5.92 ± 0.34) × 10?6, respectively, and it decreased to (5.49 ± 0.83) × 10?6 and (7.16 ± 0.73) × 10?7 at RH = 70%, respectively. Nevertheless, the HONO yields were almost independent of RH, with average values of (72 ± 3)% for the fuel-rich soot and (60 ± 2)% for the fuel-lean soot. The Langmuir-Hinshelwood mechanism was used to demonstrate the negative role of RH in the heterogeneous uptake of NO2 on soot. The species containing nitrogen formed on soot can undergo hydrolysis to produce carboxylic species or alcohols at high RH, accompanied by the release of little gas-phase HONO and NO.

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7.
Composition of exhaust from a ship diesel engine using heavy fuel oil (HFO) was investigated onboard a large cargo vessel. The emitted particulate matter (PM) properties related to environmental and health impacts were investigated along with composition of the gas-phase emissions. Mass, size distribution, chemical composition and microphysical structure of the PM were investigated. The emission factor for PM was 5.3 g (kg fuel)?1. The mass size distribution showed a bimodal shape with two maxima: one in the accumulation mode with mean particle diameter DP around 0.5 μm and one in the coarse mode at DP around 7 μm. The PM composition was dominated by organic carbon (OC), ash and sulphate while the elemental carbon (EC) composed only a few percent of the total PM. Increase of the PM in exhaust upon cooling was associated with increase of OC and sulphate. Laser analysis of the adsorbed phase in the cooled exhaust showed presence of a rich mixture of polycyclic aromatic hydrocarbon (PAH) species with molecular mass 178–300 amu while PM collected in the hot exhaust showed only four PAH masses.Microstructure and elemental analysis of ship combustion residuals indicate three distinct morphological structures with different chemical composition: soot aggregates, significantly metal polluted; char particles, clean or containing minerals; mineral and/or ash particles. Additionally, organic carbon particles of unburned fuel or/and lubricating oil origin were observed. Hazardous constituents from the combustion of heavy fuel oil such as transitional and alkali earth metals (V, Ni, Ca, Fe) were observed in the PM samples.Measurements of gaseous composition in the exhaust of this particular ship showed emission factors that are on the low side of the interval of global emission factors published in literature for NOx, hydrocarbons (HC) and CO.  相似文献   

8.
The aim of present study was for the vermiremediation of dyeing sludge from textile mill into nutrient-rich vermicompost using earthworm Eisenia fetida. The dyeing sludge was mixed with cattle dung in different ratios, i.e., 0:100 (D0), 25:75 (D25), 50:50 (D50), 75:25 (D75), and 100:0 (D100) with earthworms, and 0:100 (S0), 25:75 (S25), 50:50 (S50), 75:25 (S75), and 100:0 (S100) without earthworms. Minimum mortality and maximum population build-up were observed in a 25:75 mixture. Nitrogen, phosphorus, sodium, and pH increased from the initial to the final products with earthworms, while electrical conductivity, C/N ratio, organic carbon, and potassium declined in all the feed mixtures. Vermicomposting with E. fetida was better for composting to change this sludge into nutrient-rich manure.  相似文献   

9.
应用扫描电镜技术(SEM/EDX)对南京市两典型地区PM10中颗粒的微观形貌及其矿物组成进行了研究.结果表明,南京市大厂区(典型工业区)PM10中的颗粒多以形态规则矿物颗粒为主,山西路地区(典型商业区)PM10中的颗粒多以形态不规则出现,形态规则颗粒主要是碳酸盐、硫酸盐和铝硅酸盐矿物,形态不规则颗粒主要是烟尘结合体、生物质和原生矿物.  相似文献   

10.
Heterogeneous chemical processes involving trace atmospheric gases with solid particulates, such as carbonaceous aerosol, are not well understood. In an effort to quantify some relevant carbon aerosol systems, the heterogeneous chemistry of NO2 with both commercial and freshly prepared hexane soot was investigated in an atmospheric reaction chamber. At approximately an atmosphere of total pressure (760 Torr) and under dry conditions (relative humidities⩽1%), kinetic measurements gave an uptake coefficient of (2.4±0.6)×10−8 for n-hexane soot when referenced to the BET surface area of the sample. Commercial carbon black samples were found to yield a similar uptake coefficient. The reaction of HNO3 with commercial carbon black was also investigated and gas phase NO2 was detected as a reaction product. Low-pressure Knudsen cell experiments were carried out to facilitate a quantitative comparison between the two different techniques. The agreement between our current results and previously reported values of the uptake coefficient, with different soot samples and under varied pressure and surface coverage conditions, are discussed along with the possible implications for atmospheric chemistry.  相似文献   

11.

Singlet oxygen (1O2), hydroxyl radicals (OH), and excited triplet states of organic matter (3OM*) play a key role in the degradation of pollutants in aquatic environments. The formation rates and quantum yields (Φ) of these reactive intermediates (RI) through photosensitized reactions of dissolved organic matter (DOM) have been reported in the literature for decades. Urban biowaste-derived substances (UW-BOS), a form of organic matter derived from vegetative and urban waste, have recently been shown to be efficient sensitizers in the photo-degradation of different contaminants. Nevertheless, no quantitative measurements of photo-oxidant generation by UW-BOS have been reported. In this study, the formation quantum yields of 1O2 and OH, as well as quantum yield coefficients of TMP degradation (indicative of 3OM* formation), were quantified for two UW-BOS samples, under 254-nm UV radiation or simulated sunlight and compared to a DOM standard from the Suwanee River (SRNOM). Values of Φ for UW-BOS samples ranged from Φ(+1O2) = 8.0 to 8.8 × 10−3, Φ(+OH) = 4.1 to 4.3 × 10−6, and f TMP = 1.22 to 1.23 × 102 L Einstein−1 under simulated sunlight and from Φ(+1O2) = 1.4 to 2.3 × 10−2, Φ(+OH) = 1.3 to 3.5 × 10−3, and f TMP = 3.3 to 3.9 × 102 L Einstein−1 under UV. Although UW-BOS are not necessarily better than natural DOM regarding photosensitizing properties, they do sensitize the production of RI and could potentially be used in engineered treatment systems.

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12.
Vehicle particle emissions are studied extensively because of their health effects, contribution to ambient PM levels and possible impact on climate. The aim of this work was to obtain a better understanding of secondary particle formation and growth in a diluting vehicle exhaust plume using 3-d information of simulations together with measurements. Detailed coupled computational fluid dynamics (CFD) and aerosol dynamics simulations have been conducted for H2SO4–H2O and soot particles based on measurements within a vehicle exhaust plume under real conditions on public roads.Turbulent diffusion of soot and nucleation particles is responsible for the measured decrease of number concentrations within the diesel car exhaust plume and decreases coagulation rates. Particle size distribution measurements at 0.45 and 0.9 m distance to the tailpipe indicate a consistent soot mode (particle diameter Dp∼50 nm) at variable operating conditions. Soot mode number concentrations reached up to 1013 m−3 depending on operating conditions and mixing.For nucleation particles the simulations showed a strong sensitivity to the spatial dilution pattern, related cooling and exhaust H2SO4(g). The highest simulated nucleation rates were about 0.05–0.1 m from the axis of the plume. The simulated particle number concentration pattern is in approximate accordance with measured concentrations, along the jet centreline and 0.45 and 0.9 m from the tailpipe. Although the test car was run with ultralow sulphur fuel, high nucleation particle (Dp⩽15 nm) concentrations (>1013 m−3) were measured under driving conditions of strong acceleration or the combination of high vehicle speed (>140 km h−1) and high engine rotational speed (>3800 revolutions per minute (rpm)).Strong mixing and cooling caused rapid nucleation immediately behind the tailpipe, so that the highest particle number concentrations were recorded at a distance, x=0.45 m behind the tailpipe. The simulated growth of H2SO4–H2O nucleation particles was unrealistically low compared with measurements. The possible role of low and semi-volatile organic components on the growth processes is discussed. Simulations for simplified H2SO4–H2O–octane–gasoil aerosol resulted in sufficient growth of nucleation particles.  相似文献   

13.
Abstract

The mobility of seven pesticides in a chromic cambisol soil was studied by soil thin layer chromatography. Pesticide mobilities were determined by means of conventional autoradiographs of the chromatograms, as well as from sequential series of curves and images of the pesticide spots provided by a linear analyser. The R f values obtained from the autoradiographs and those provided by the linear analyser were quite consistent. Based on such values, pesticide mobility decreased in the following order: acephate > fluometuron > atrazine > ethofumesate > metolachlor > diazinon > glyphosate. According to the mobility scale proposed by Helling and Turner (1968), acephate is highly mobile; atrazine, fluometuron, ethofumesate and metolachlor are moderately mobile; diazinon is slightly mobile; and glyphosate is immobile. The images provided by the linear analyser allow to determine the R f values for the zones of maximum activity in the pesticide spots (R f max), as well as the activities of different spot zones and those corresponding to R f and R f max. The results obtained show the image analyser to provide more expeditious R f measurements from the chromatograms and open up new prospects for using soil TLC to investigate pesticide mobility.  相似文献   

14.
The influence of 222Rn exhalation from walls and air exchange (low ventilation rates ν<0.3 h-1) upon its concentration in room air has been considered. It was found that the radon concentration reachs 84 Bq m-3 at exhalation and ventilation rates of 66 Bq hm-2 and 0.28 h-1, respectively. The radon concentration and the ultrafine fraction fp of potential α energy concentration as well as the equilibrium factor F of the short-lived radon progeny were also determined in three different completely closed rooms. An electroprecipitation method was applied for determining the 222Rn concentration while a single wire-screen technique was used for the determination of ultrafine radon progeny. During the measurements, the radon concentrations were varied between 33 and 134 with a mean value 89 Bq m-3. A mean ultrafine fraction (fp) of 0.16 was obtained at a mean aerosol particle concentration (Z) of 1700 cm-3 and a mean equilibrium factor (F) of 0.33. The obtained mean value of fp was found to be about five times higher than the value reported in the ICRP publication (fp=0.03). The attachment rate (X), the deposition rate (qf) and the deposition velocity (vfd) of the ultrafine radionuclide 218Po were calculated. A mean value of X was found to be 49 h-1 at a mean qf of 46 h-1 and a mean vfd of 4.6 m h-1. The attachment coefficient β of 218Po was found to vary between 0.016 and 0.047 with a mean value 0.028 cm3 h-1.  相似文献   

15.
Using the relative technique, rate coefficients have been measured for the gas phase reactions of hydroxyl radicals with four fluoroacetates, methyl trifluoroacetate (CF3COOCH3), ethyl trifluoroacetate (CF3COOCH2CH3), methyl difluoroacetate (CF2HCOOCH3) and 2,2,2-trifluoroethyl trifluoroacetate (CF3COOCH2CF3). Experiments were carried out at 296±2 K and atmospheric pressure (∼750 Torr) using nitrogen or synthetic air as bath gases. The following rate coefficients were derived for the reaction of OH radicals (in units of cm3 mol−1 s−1) with CF3COOCH3, k=(4.97±1.04)×10−14, CF3COOCH2CH3, k=(2.64±0.59)×10−13, CF2HCOOCH3, k=(1.48±0.34)×10−13 and CF3COOCH2CF3, (1.05±0.23)×10−13. The rate constants obtained are compared with previous literature data of other volatile organic compounds to establish reactivity trends. Atmospheric implications are discussed in terms of lifetimes and fates of the fluoroacetates in the troposphere.  相似文献   

16.
A novel photocatalytic reactor for wastewater treatment was designed and constructed. The main part of the reactor was an aluminum tube in which 12 stainless steel circular baffles and four quartz tube were placed inside of the reactor like shell and tube heat exchangers. Four UV–C lamps were housed within the space of the quartz tubes. Surface of the baffles was coated with TiO2. A simple method was employed for TiO2 immobilization, while the characterization of the supported photocatalyst was based on the results obtained through performing some common analytical methods such as X-ray diffraction (XRD), scanning electron microscope (SEM), and BET. Phenol was selected as a model pollutant. A solution of a known initial concentration (20, 60, and 100 ppmv) was introduced to the reactor. The reactor also has a recycle flow to make turbulent flow inside of the reactor. The selected recycle flow rate was 7?×?10?5 m3.s?1, while the flow rate of feed was 2.53?×?10?7, 7.56?×?10?7, and 1.26?×?10?6 m3.s?1, respectively. To evaluate performance of the reactor, response surface methodology was employed. A four-factor three-level Box–Behnken design was developed to evaluate the reactor performance for degradation of phenol. Effects of phenol inlet concentration (20–100 ppmv), pH (3–9), liquid flow rate (2.53?×?10?7?1.26?×?10?6 m3.s?1), and TiO2 loading (8.8–17.6 g.m?2) were analyzed with this method. The adjusted R 2 value (0.9936) was in close agreement with that of corresponding R 2 value (0.9961). The maximum predicted degradation of phenol was 75.50 % at the optimum processing conditions (initial phenol concentration of 20 ppmv, pH?~?6.41, and flow rate of 2.53?×?10?7 m3.s?1 and catalyst loading of 17.6 g.m?2). Experimental degradation of phenol determined at the optimum conditions was 73.7 %. XRD patterns and SEM images at the optimum conditions revealed that crystal size is approximately 25 nm and TiO2 nanoparticles with visible agglomerates distribute densely and uniformly over the surface of stainless steel substrate. BET specific surface area of immobilized TiO2 was 47.2 and 45.8 m2 g?1 before and after the experiments, respectively. Reduction in TOC content, after steady state condition, showed that maximum phenol decomposition occurred at neutral condition (pH?~?6). Figure
The schematic view of the experimental set-up  相似文献   

17.

In order to improve and establish the localized source profile of PM2.5 in Fuxin, the ashes under dust catcher were collected from four typical coal-fired power plants in Fuxin and twenty-eight components were measured. The source profile of PM2.5 in the soot of the four coal-fired power plants was established. SO42? was the most abundant component in the PM2.5 of the soot of the four coal-fired power plants, followed by Ca2+ and organic carbon (OC). The content of element components in PM2.5 smoke ranges from 5.06 to 10.97%, the content of ionic components ranges from 36.53 to 48.59%, and the total carbon content ranges from 9.43 to 11.36%. The divergence coefficient of PM2.5 source profile in Fuxin coal burning smoke is mostly similar to that of Fushun, whereas the divergence coefficient of Colorado reaches 0.65, indicating that Fuxin coal burning power plant smoke has no similarity to Colorado. The order of the geological accumulation index of Ni, Cu, V, Mn, and Cr was Cr (4.58) > Mn (4.42) > V (4.38) > Cu (4.09) > Ni (4.06), showing a heavy pollution level. The health risk assessment model recommended by the USEPA was used to assess the health risk of heavy metals in soot of coal-fired power plants, and the non-carcinogenic risk values of As for children and adults were 45.7 and 4.90, respectively. The carcinogenic risk values of Cr for adults and children were the highest, with values of 3.66 × 10?5 and 2.06 × 10?5, respectively, followed by As.

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18.
Much rain and strong winds caused by a cold front occurred in Beijing during the period of Sep. 27 to Oct. 4, 2004 and led to sharp drops in maximum and mean concentrations of HONO, HCHO, O3, and NO2, i.e., the maximum concentrations were reduced by 5.9, 21.3, 45.6, and 44.4 ppb, respectively, and the mean concentrations were decreased by 4.0, 5.5, 30.3, and 32.3 ppb, respectively. For daily HOx production rates HONO photolysis was the largest contributor and over 90% contributions were from photolysis of HONO and HCHO. Large number and area percentages of soot aggregate from PM10, and high correlations between concentrations of PM10 and chemical formation of HONO suggested that heterogeneous reactions of NO2 on surfaces of soot aggregate could be a key source of HONO in the heavy traffic areas of Beijing during the night and should be considered in air quality simulations for such areas.  相似文献   

19.
Koelmans AA  Jonker MT 《Chemosphere》2011,84(8):1150-1157
It is unknown whether carbonaceous geosorbents, such as black carbon (BC) affect bioturbation by benthic invertebrates, thereby possibly affecting sediment-water exchange of sediment-bound contaminants. Here, we assess the effects of oil soot on polychlorinated biphenyl (PCB) mass transfer from sediment to overlying water, for sediments with and without tubificid oligochaeta as bioturbators. PCB levels were so low that toxicity to the oligochaeta played no role, whereas soot levels and binding affinity of PCBs to soot were so low that pore water PCB concentrations were not significantly affected by binding of PCBs to soot. This setup left direct effects of BC on bioturbation activity as the only explanation for any observed effects on mass transfer. Mass transfer coefficients (KL) for benthic boundary layer transport were measured by a novel flux method using Empore™ disks as a sink for PCBs in the overlying water. For the PCBs studied (logKow 5.2-8.2), KL values ranged from 0.2 to 2 cm × d−1 in systems without tubificids. Systems with tubificids showed KL values that were a factor of 10-25 higher. However, in the presence of oil soot, tubificids did not cause an increase in mass transfer coefficients. This suggests that at BC levels as encountered under field conditions, the mechanism for reduction of sediment-water transfer of contaminants may be twofold: (a) reduced mass transfer due to strong binding of the contaminants to BC, and (b) reduced mass transfer of contaminants due to a decrease in bioturbation activity.  相似文献   

20.
Characteristic parameters of black carbon aerosol (BC) emitted from jet engine were measured during ground tests and in-flight behind the same aircraft. Size distribution features were a primary BC mode at a modal diameter D≈0.045 μm, and a BC agglomeration mode at D<0.2 μm. The total BC number concentration at the engine exit was 2.9×107 cm-3 with good agreement between model results and in-flight measured number concentrations of non-volatile particles with D⩾0.014 μm. A comparison between total number concentration of BC particles and the non-volatile fraction of the total aerosol at the exit plane suggests that the non-volatile fraction of jet engine exhaust aerosol consists almost completely of BC. In-flight BC mass emission indices ranged from 0.11 to 0.15 g BC (kg fuel)-1. The measured in-flight particle emission value was 1.75±0.15×1015 kg-1 with corresponding ground test values of 1.0–8.7×1014 kg-1. Both size distribution properties and mass emission indices can be scaled from ground test to in-flight conditions. Implications for atmospheric BC loading, BC and cirrus interaction and the potential of BC for perturbation of atmospheric chemistry are briefly outlined.  相似文献   

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