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1.
Abstract

The removal of sulfur dioxide (SO2) from simulated flue gases streams (N2/O2/H2O/SO2) was experimentally investigated using microgap discharge. In the experiment, the thinner dielectric layers of aluminum oxide (Al2O3) were used to form the microgap discharge. With this physical method, a high concentration of hydroxyl (OH·) radicals were produced using the ionization of O2 and H2O to further the conversion of SO2 into sulfuric acid (H2SO4) at 120° C in the absence of any catalysts and absorbents, which were captured with the electrostatic precipitator (ESP). As a result, the increase of discharge power and concentrations of O2 and H2O increased the production of OH· radicals resulting in enhanced removal of SO2 from gas streams. With the test and analysis, a number of H2SO4 droplets were produced in experiment. Therefore, a new method for removal of SO2 in semidry method without ammonia (NH3) additive was found.  相似文献   

2.
Leaf injury data from acute and chronic exposure studies of Dare soybean were regressed against the logarithms of exposure time and O3 and SO2 concentrations to develop a new two-pollutant leaf injury model (which explains 88% of the variance) and to calculate the parameters of best fit for this new model and a previously developed one-pollutant model. Using the calculated parameters, the percentage of leaf surface Injured over a growing season by O3, SO2, or both simultaneously was estimated for an ambient air sampling site located 2 miles from a coal burning power plant. For this site, the one- and two-pollutant models predicted that SO2 effects would be negligible If SO2 concentrations never exceeded the National Ambient Air Quality Standard (NAAQS) of 0.50 ppm, averaged over 3 h. However, calculations suggest that O3 may injure up to 24% of Dare soybean leaf surface over a growing season even though the O3 NAAQS of 0.12 ppm, averaged over 1 h, is never exceeded. Because the 3 h SO2 standard is exceeded at very few places, the O3 model is usually sufficient to estimate Dare soybean leaf Injury. Leaf injury is estimated by taking the logarithm of the summation of each daytime hour’s exponentiated O3 concentration (c) measured at an ambient air sampling site over a growing season. This is expressed as: z = -0.0828 + 0.4876 in (Σco3 2.618), where z is the Gaussian transform of percent leaf injury. The methods developed in this paper, using Dare soybean data as an example, may apply to other plants.  相似文献   

3.
The washout coefficient of a gas in air is the fraction of it removed in unit time by rain below cloud base. The ‘apparent’ coefficients were estimated by statistically comparing hourly ground-level concentrations just before and at the onset of heavy, non-frontal rain. The concentrations were obtained from 5 y of continuous monitoring at a rural site.The coefficient (s−1) estimated for SO2 was (2.61 ± 0.14) × 10−5 times the rate of rainfall (mm h −1). This is completely consistent with a previously published value derived from the data from 10 rural sites for one year, and both estimates are consistent with published values of dissolved SO2 in rainwater at another rural site, giving some confidence in the technique.The values of the coefficients estimated for NO and NO2 were about 40 and 80%, respectively of that for SO2. Some nitrite is found in rainwater, but not enough to explain the washout found. However, the analysers used would measure HNO3 aerosols as NO2, and these are very soluble. In addition, fast reactions are known which can convert oxides of nitrogen into soluble nitrates, present in sufficient concentration in rainwater.The statistical process leads to the coefficient estimated for O3 being negative, implying that O3 is produced at the time of rain. This is most probably due to the strong winds and turbulence which accompany heavy rain, giving replenishment of low-level O3 from upper air levels where O3 is normally produced. No systematic changes in the other gas concentrations accompany the changes in O3 values.  相似文献   

4.
A comprehensive ‘operational’ evaluation of the performance of the Community Multiscale Air Quality (CMAQ) modelling system version 4.6 was conducted in support of pollution assessment in the UK for the calendar year 2003. The model was run on multiple grids using one-way nests down to a horizontal resolution as fine as 5 km over the whole of the UK. The model performance was evaluated for pollutants with standards and limit values (e.g. O3, PM10) and species contributing to acidic and nitrogenous deposition (e.g. NH3, SO42–, NO3, NH4+) against data from operational national monitoring networks. The key performance characteristics of the modelling system were found to be variable according to acceptance criteria and to depend on the type (e.g. urban, rural) and location of the sites, as well as on the time of the year. As regards the techniques that were used for ‘operational’ evaluation, performance generally complied with expected levels and ranged from good (e.g. O3, SO42–) to moderate (e.g. PM10, NO3). At a few sites low correlations and large standard deviations for some species (e.g. SO2) suggest that these sites are subject to local factors (e.g. topography, emission sources) that are not well described in the model. Overall, the model tends to over predict O3 and under predict aerosol species (except SO42–). Discrepancies between predicted and observed concentrations may be due to a variety of intertwined factors, which include inaccuracies in meteorological predictions, chemical boundary conditions, temporal variability in emissions, and uncertainties in the treatment of gas and aerosol chemistry. Further work is thus required to investigate the respective contributions of such factors on the predicted concentrations.  相似文献   

5.
Calibration gas standards for H2S, CH3SH, CS2 and SO2, independently prepared by two separate research groups from the University of Idaho Department of Chemistry and the NOAA Aeronomy Laboratory, were directly intercompared using a gas chromatographic-flame photometric measurement procedure for all four species and a fluorimetric measurement procedure for H2S. The NOAA gas standard system used gravimetrically-calibrated ‘low loss’ permeation tubes in conjunction with a three-stage dynamic dilution system. The University of Idaho (UI) system used single-stage dilution of the effluent from ‘ultra-low loss’ permeation tubes, which were calibrated by a metal foil collection/flash desorption/flame photometric detection procedure using aqueous sulfate standards. Comparative measurements between UI and NOAA gas standards in the 1–2 ppbv range showed differences no greater than 12 % for CS2, SO2 and CH3SH, and 21 % for H2S.  相似文献   

6.
Historically, studies of the effects of the main phytotoxic gases (SO2, O3, NOx and HF) have focused on determining the threshold for onset of visible foliar injury. The current U.S.A. air quality standards to protect vegetation (500 ppb SO2 for 3 h and 120 ppb O3 for l h not to be exceeded more than once per annum) are good examples of the use of this information in the regulatory process. More recently, research has focused on determining the thresholds for effects on economically important yield parameters irrespective of foliar injury. The implication is that long-term seasonal or annual standards may be required to prevent yield losses particularly for the primary pollutants in diffuse-source regions and for secondary pollutants. This paper reviews the literature on thresholds for yield effects of SO2 and O3 and concludes that
  • 1.(a) the current EEC standard for SO2 is adequate to protect most crops and trees and
  • 2.(b) more work is required to determine whether the U.S.A. threshold for O3 effects are applicable to the climate and crops of Europe.
Recent results suggest that yield responses vary so much with climatic factors that broad regional standards may not be acceptable. In addition, the effect of one phytotoxic gas must now be assessed against the background of the other gases.Future research on effects of SO2 and O3 in particular, will be increasingly influenced by the use of cost-benefit analysis in the regulating process and the consequent demand for dose-response relationships. This approach is fraught with difficulty and particular problems arise
  • 1.(a) when ‘hypothetical’ relationships are assumed in the absence of good data and
  • 2.(b) when the linearity of dose-response relationships are presumed to justify the extrapolation from effects at high concentrations to lower ambient concentrations.
The evidence for nutritional effects of low levels of SO2 and NOx abrogates this assumption and suggests that for some gases at least, there should be a threshold below which no detrimental effects occur. This paper reviews the recent work aimed at producing dose-response relationships for economically important yield parameters.  相似文献   

7.
The frequency of co-occurrences for SO2NO2, SO2/O3 and O3/NO2 at rural and remote monitoring sites in the United States was characterized for the months of May-September for the years 1978–1982. Minimum hourly concentrations of 0.03 and 0.05 ppm of each gas were used as the criteria for defining a ‘co-occurrence’. The objectives of this study were to:
  • 1.(1) identify the types of co-occurrence patterns and their frequency;
  • 2.(2) identify whether the frequency of hourly simultaneous co-occurrences increased substantially when the minimum concentration was lowered (e.g. from 0.05 to 0.03 ppm) for each pollutant; and
  • 3.(3) determine whether the frequency of co-occurrences showed large year-to-year variation.
For all pollutant pairs and co-occurrence thresholds (i.e. 0.03 and 0.05 ppm), the frequency of daily and hourly co-occurrences was low for most sites. Year-to-year variability was found to be insignificant; most of the monitoring sites experienced co-occurrences of any type less than 12% of the 153 days. Based on our observations, researchers attempting to assess the potential effects of SO2/NO2, SO2/O3 and O3/NO2 in the United States should construct simulated exposure regimes so that
  • 1.(1) hourly simultaneous and daily simultaneous-only co-occurrences are fairly rare and
  • 2.(2) when co-occurrences are present, complex-sequential and sequential-only co-occurrence patterns predominate.
  相似文献   

8.
Besides well-known episodic Kosa during spring, high concentrations of Ca2+ in aerosols were observed early in summer as well as in the semi-continuous data of the aerosols at the summit of Mt. Fuji. We further analysed the data to study the chemical characteristics of the high calcium event during early summer. The back trajectory analyses of the event indicated that Ca was transported from arid and semi-arid regions (e.g. the Taklamakan desert) through the westerly-dominated troposphere higher than the height of the summit of Fuji. The amount of SO42? was always equivalent to that of NH4+ unlike the case of the normal Kosa period where SO42? is in excess with respect to NH4+. This shows the ‘after’ mixing of unreacted CaCO3 of Kosa origin with (NH4)2SO4, which was only realized by the downward injection of Kosa particles from higher altitudes to the air masses of different origin. In the case of normal Kosa, the air bearing Kosa particles passed through the polluted area to absorb unneutralized acids (‘on-the-way’ mixing), whereas in the case of the Kosa-like phenomena in summer, the acids from the polluted area have been neutralized by NH4+ and become inactive before mixing with CaCO3 (“after” mixing). We have simplified the chemistry of aerosols using their three major components, Ca2+, SO42? and NH4+, and introduced a new triangle diagram with the three assumed end-members of CaCO3, CaSO4 and (NH4)2SO4 to quantify the contribution of the ‘after’ mixing to the aerosols (AMI; ‘after’ mixing index). Based on the back trajectories of some high AMI cases, CaCO3 in Kosa particles was transported through the middle troposphere (5000–7000 m) and descended to meet another air mass where SO42? had been already neutralized by NH3.  相似文献   

9.
Poplar shoots were exposed for 3–4 weeks to filtered air, ambient (maximum values 50–60 nl -1) or two times ambient O3-concentrations under controlled environmental conditions in fumigation chambers. A sensitive (Populus nigra ‘Brandaris’) and a tolerant (P. euramericana ‘Robusta’) cultivar were used. At regular intervals the uptake of O3, transpiration and CO2 assimilation rate (Pn) of full-grown leaves were measured with leaf cuvettes. For unaffected leaves, the measured flux of O3 into the leaves appeared to be larger than can be calculated using the stomatal conductance for O3 (gs,o) estimated from the transpiration rates of the same leaves. Resistance analysis revealed that the difference was partly a result of a reaction with the external leaf surface. However, when the O3 flux into the leaf was corrected for this reaction, it was still larger than can be estimated using gs,o. As a consequence, negative residual or internal resistances (ri) for O3 transport into the leaves were assessed. It is postulated that O3 molecules moving into the leaf follow a shorter pathway than effluxing H2O-molecules. P. ‘Brandaris’ leaves showed a reduction in Pn after 12 days of exposure to ambient O3-concentrations, whereas for P. ‘Robusta’ a reduction in Pn was only observed at two times ambient concentrations. A simultaneous decline in the O3-flux was found in both cases. The decline occurred before a decrease in gs,o was observed suggesting that the O3 flux into the affected leaves was first hindered by internal factors. The measured flux of the affected leaves became smaller than the flux estimated using gs,o and, consequently, positive ri-values were estimated. The change in ri suggests that O3 molecules not only penetrated deeper into the leaf, but also were accumulating at a prolonged exposure. Our results indicate that ri may be a potentially important component of the overall resistance for O3-uptake, which may have important consequences for estimating O3 uptake from water vapour flux data.  相似文献   

10.
The information presented in this paper is directed to engineers who are involved with environmental emissions from coal conversion plants. Synthetic sorbents were investigated as an alternative to natural sorbents (limestone) for the removal of SO2 from the combustion gas in a fluidized-bed coal combustor. The sulfation rate of a synthetic sorbent, CaO in α-AI2O3, was determined as a function of gas composition, temperature, and calcium concentration in the sorbent. The reaction was found to be diffusion-controlled above 850°C and kinetically controlled at lower temperatures. The physical characteristics of the support material have a major effect oh the sulfation kinetics. Porosity measurements indicated that supports containing large pores (>0.2 µm) produced sorbents having high sulfation rates and that pores with diameters less than 0.2 µm did not contribute significantly to the capture of SO2. The sorbents SrO in α-AI2O3 and BaO in α-AI2O3 had lower SO2 capture rates than did CaO in α-AI2O3. The alkali metal oxide sorbents K2O and Na2O in α-AI2O3 captured SO2 much faster than did the alkaline earth metal oxides.  相似文献   

11.
Ten species of plants, five perennials and five annuals, native to the Mojave desert were grown in pots and fumigated in open top plastic greenhouses, 25 hours/week, with SO2 and/or NO2. Three levels of SO2: 2.0, 0.67, and 0.22 parts per million (ppm); three levels of NO2: 1.0, 0.33, and 0.11 ppm; three treatments with 2.0 ppm SO2 + 1.0 ppm NO2, 0.67 ppm SO2 + 0.33 ppm NO2 and 0.22 ppm SO2 + 0.11 ppm NO2 plus untreated control plants were used in the fumigations. The perennials were fumigated for 16 weeks in 1977 and 32 weeks in 1978. Three species of annuals were grown and fumigated for 17 weeks, a fourth for 16 weeks, and a fifth for 12 weeks. A second crop of the first three annuals were grown; one for 12 weeks, a second for 8, and a third for 9 weeks.

Individual species differed widely in their particular responses to the fumigants. The fumigations of perennials with 2.0 ppm of SO2 or NO2 at 1.0 ppm caused extensive leaf injury, and reduced growth or dry weight of Larrea divaricate Cav., Chilopsls linearis Cav., and Ambrosia dumosa (Gray) Payne. The combined fumigants had additive effects. No suggestion of synergism was noted. These fumigants at lower concentrations stimulated lateral growth of Encelia farinosa Gray ex Torr. and Erodium cicutarium (L.) L’Her., dry weight of Atriplex canescens (Pursh) Nutt. and Plantago insularis Eastw. and increased flowering of Balleya pleniradiata Harv. and Gray, thus indicating beneficial effects.

Annual species were more severely affected by 2.0 ppm SO2 than the perennials and extensive injury or death of plants occurred in all annuals. At the 0.67 ppm level severe leaf injury occurred. NO2 at 1.0 ppm was less injurious than SO2 and addition of NO2 to SO2 suggested an antagonistic effect. Plant survival and flowering was increased by adding NO2 to plants being treated with SO2

Comparison of perennial species showed Larrea sensitive, Chilopsis, Encella and Ambrosia intermediate, and Atriplex resistant. The annual species showed Erodium cicutarium and Plantago Insularis to be extremely sensitive, Phacelia crenulata Torr very sensitive and Baileya pleniradiata sensitive. Chaenactis carphoclinia Gray grew poorly and no valid rating was possible.  相似文献   

12.
The synoptic climatology of ozone (O3) for S Ontario has shown that, over the 1976–1981 period, average summer O3 concentrations follow a relationship similar to that reported for event analysis during periods of high O3 concentration. Highest average concentrations, 36 parts per billion (ppb), occur with ‘back of the high’ situations while lowest average concentrations (20 ppb) occur with ‘front of the high’ situations.With similar weather events in the winter, the pattern is reversed with highest average O3 concentrations on the ‘front of the high’ (19 ppb) and lowest average concentrations on the ‘back of the high’ (13 ppb). Concentration of O3 in the ‘front of the high’ sector is due in part to the intrusion of O3 in the vicinity of storms from the stratosphere. The seasonal variation of average concentrations in these situations is low, ranging from 14 to 26 ppb.The very low average concentration during the winter and fall for the ‘back of the high’ situation may be the result of scavenging by NOx from the urban/industrial areas around the Great Lakes. During the spring and summer, solar energy and warm temperatures cause the photochemical production of O3 from NOx and HCs precursors. In the fall and winter, photochemical production of O3 is either very low or absent, and the NOx consume O3 rather than produce it. Thus, average O3 concentrations for winter ‘back of the high’ situations are one-third of those in the summer months.The synoptic climatology of events during the months from May to September with maximum O3 concentrations in excess of 80 ppb indicates that 78 % of these events occur under synoptic weather classes generally indicative of back or centre of the high situations.  相似文献   

13.
Concentrations of 23 elements plus NO3, SO42− and Cl were determined for samples collected continuously every 3 or 6 h during 22–27 July, 1985 at a suburban site in Karachi, Pakistan. Concentrations of lithophilic elements and several anthropogenic elements were ~ 80 % higher during daytime than at night. These elevated levels were attributed to daytime increases in wind velocity and anthropogenic activity. Factor analysis showed that ~ 50% of the variance was associated with soil, and ~ 14 % each with oceanic Na and Cl, anthropogenic Sb and Pb, and Zn, Se and SO42−. A cement (limestone/dolomite) factor was not separated even though Ca and Mg concentrations were unusually high and a cement factory was located nearby. This led to an investigation of a chemical approach to determine the sources. Concentrations of Na, Mg and Ca were determined in water-extracts of the samples. Assuming soluble Na (~ 92 % of total) to be sea derived, marine components of Mg, SO42−, Ca and Br were determined. Solubility considerations were then used to reveal the cement source and apportion the aerosol sources. On the average, approximately 48 % of the total aerosol mass could be accounted for by the ‘cement’ and ‘soil’ components; about 12 % by the ‘sea salt’, about 3% by the ‘fossil fuel’ SO42− (as (NH4)2SO4); about 1 % by the NO3 (as NH4NO3); the remaining 36 % of the aerosol mass was unassigned.  相似文献   

14.
Cucumber and bean plants were pretreated with different SO2 concentrations for various lengths of time and subsequently exposed to an injurious O3 exposure. In cucumber, increasing levels of SO2 and increasing length of pre-exposure progressively enhanced O3 injury. In bean O3 sensitivity progressively decreased with both increasing SO2 concentration and length of pre-exposure. The effect of SO2 was not related to measurable increases in tissue S content. SO2 concentrations as low as 20 ppb can increase O3 sensitivity in cucumber.  相似文献   

15.
Biochemical and physiological experiments were conducted on pea plants (Pisum sativum) continuously exposed in growth chambers to SO2 gas for 18 days. S02 gas concentrations were 0.1, 0.15, and 0.25 ppm. In plants exposed to 0.1 and 0.15 ppm it was clearly demonstrated that there was a greater accumulation of inorganic sulfur, a reduced buffer capacity of the cells relative to H-ions, and a stimulation of glutamate dehydrogenase activity. The only macroscopic symptom seen was slight chlorosis of the older leaves. There was only a slight decrease in fresh and dry weights of these plants compared to the control plants whereas in the group of plants exposed to 0.25 ppm SO2 foliage necrosis was considerable. In addition, there was a marked reduction in the fresh and dry weights of the latter plants. However, the relationship among accumulated inorganic sulfur, reduced buffer capacity, and increased glutamate dehydrogenase activity as seen for the lower S02 concentrations was close. Accordingly, if might be possible to use these three parameters to diagnose S02 injury before any significant symptoms appear. In the case of severe SO2 injury there was a marked increase in glutamine and ammonia concentrations suggesting that these factors in addition to the above could be used in diagnosing severe SO2 injury. There was no significant difference between plants treated with 0.1 or 0.15 ppm SO2 and control plants in the contents of K, Ca, P, and N fractions. Therefore, these factors would not be useful in the early detection of SO2 injury.  相似文献   

16.
SO2/O2 mixtures were photolyzed at 3130 Å and in the range 2500–4000 Å at room temperature. The only product of photolysis was SO3. Attempts to estimate ф(S03) using mass spectrometry, l.R. spectroscopy and pressure change measurements were unsuccessful, because it was not possible to obtain reproducible quantitative estimates of SO3. ф(SO2) values were determined by monitoring the 3130 Å absorption for its concentration measurements. ф(SO2) was independent of SO2 (11.6 to 50.4 torr) and O2 (50.0 to 390.6 torr) pressures. At 3130 Å, ф(SO2) varied between 1.5 × 10?2 and 2.2 X 10?2. Over the integrated range 2500–4000 Å ф(SO2) values of 2.1 X 10?3 to 2.9 X 10?3 were obtained. The differences in ф(SO2) values are explained in terms of wavelength dependence of the rate constants for the two primary reactions: 1SO2 + SO2 → 2SO2(1) and 1SO2 + SO23SO2 + SO2(2); (k2/k1) 3130 Å ≈ 10(k2/k1)2500–4000 Å.  相似文献   

17.
The sensitivity of in-cloud oxidation of SO2 in corrective clouds to a number of chemical and physical parameters is examined. The parameterization of precipitation growth processes is based on the work of Scott (1978) and Hegg (1983). A chemical model predicts gas and aqueous phase distributions of soluble gases and in-cloud uncatalyzed oxidation of SO2 by O3 and H2O2. Sulfate aerosol and SO2, CO2, NH3, H2O2 and O3 gases and their aqueous phase dissociation products are treated.The results indicate that in-cloud conversion is an important removal mechanism for SO2 and accounts for a significant fraction of the precipitation sulfate. However, except at low SO2 concentrations, the precipitation sulfate concentration is insensitive to the initial SO2 concentration; the sulfate concentration is most sensitive to the initial H2O2 and NH3 concentrations. At low SO2 concentrations, the precipitation sulfate concentration is determined primarily by the initial sulfate aerosol concentration. The feedback between sulfate production and pH is important in limiting SO2 oxidation by O3. If gas phase H2O2 of order 1 ppb is the major source of aqueous phase H2O2 for S(IV) oxidation, it is likely that the oxidation reaction is oxidant limited. The sulfate concentration is a decreasing function of the precipitation rate. At low rainfall rates (< 1 mm h−1), ice phase growth decreases the sulfate concentration. However, the results are insensitive to an ice phase origin at moderate and high rainfall rates.  相似文献   

18.
Studies of the dispersion of pollutants (SO2, O3) in the planetary boundary layer have been performed during the Fos Berre 1983 International Campaign using ground-based DIAL lidar operating in the u.v. wavelength range. Multidimensional measurements of both SO2 and O3 were obtained with a spatial resolution better than 500 m, a temporal resolution of 3 mn and a maximum horizontal range of 3 km. The overall accuracy as assessed by various comparisons with other measurement systems was always better than 20%. Examples of application to studies of SO2 dispersion in the planetary boundary layer, of plume evolution and of horizontal inhomogeneities in the ozone field are given.  相似文献   

19.
With rising concentrations of both atmospheric carbon dioxide (CO2) and tropospheric ozone (O3), it is important to better understand the interacting effects of these two trace gases on plant physiology affecting land-atmosphere gas exchange. We investigated the effect of growth under elevated CO2 and O3, singly and in combination, on the primary short-term stomatal response to CO2 concentration in paper birch at the Aspen FACE experiment. Leaves from trees grown in elevated CO2 and/or O3 exhibited weaker short-term responses of stomatal conductance to both an increase and a decrease in CO2 concentration from current ambient level. The impairement of the stomatal CO2 response by O3 most likely developed progressively over the growing season as assessed by sap flux measurements. Our results suggest that expectations of plant water-savings and reduced stomatal air pollution uptake under rising atmospheric CO2 may not hold for northern hardwood forests under concurrently rising tropospheric O3.  相似文献   

20.
Sodium thiosulfate (Na2S2O3) has been tested in a pilot plant as an oxidation inhibitor in flue gas desulfurization by lime and limestone slurry scrubbing with and without MgO and adiplc acid additives. The effectiveness of thiosulfate is proportional to the inhibitor product, defined as the product of thiosulfate concentration (M), calcium concentration (M), and the moles of SO2 absorbed per hour per liter of hold tank volume. Gypsum saturation was less than 100 percent and scaling was eliminated when the inhibitor product exceeded 0.3 × 10?6(gmol/L)3/h. Thiosulfate was relatively more effective in systems with chlorides and less effective in systems promoted by MgO. An inhibitor product greater than 10?6(gmol/L)3/h significantly enhanced dewatering of solids from limestone scrubbing. SO2 removal and/or limestone utilization were increased in systems that started with less than 10 mM dissolved calcium.  相似文献   

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