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1.
The body of Information presented in this paper is directed to those Individuals concerned with the removal of NOx in combustion flue gases. A catalytic process for the selective reduction of nitrogen oxides by ammonia has been investigated. Efforts were made toward the development of catalysts resistant to SOx poisoning. Nitrogen oxides were reduced over various metal oxide catalysts in the presence or absence of SOx(SO2 and SO3). Catalysts consisting of oxides of base metals (for example, Fe2O3) were easily poisoned by SO3, forming sulfates of the base metals. A series of catalysts which are not susceptible to the SOx poisoning has been developed. The catalysts possess a high activity and selectivity over a wide range of temperatures, 250—450°C. The catalysts were tested in a pilot plant which treated a flue gas containing 110-150 ppm NOx, 660-750 ppm SO2, and 40-90 ppm SO3. The pilot plant was operated at 350°C and at a space velocity of 10,000 h-1. The removal of nitrogen oxides was more than 90% for several months.

A mechanism of the NO-NH3 reaction has also been investigated. It is found that NO reacts with NH3 at a 1:1 mole ratio in the presence of oxygen and the reaction is completely inhibited by the absence of oxygen. The experimental data show that the NO-NH3 reaction in the presence of oxygen is represented byNO + NH3 + 1/4 O2 = N2 + 3/2 H2O.  相似文献   

2.
The breakthrough curve for NO adsorption on the activated carbon fibers treated in iron salt solutions was determined. They can adsorb much more NO than granular activated carbon by a factor of more than 10 from a flowing 300 ppm NO-N2 mixed gas at 100°C and 20 ml min−1; the most effective one of the iron-treated carbon fibers of 0.2 g is able to reduce the NO concentration from 300 ppm to 30 ppm. These adsorbents can adsorb the same amount of NO from even a 300 ppm NO-500 ppm SO2-10% CO2-10% H2O-1% O2-N2 mixed gas.  相似文献   

3.
Salinity increases mobility of heavy metals in soils   总被引:11,自引:0,他引:11  
The effect of salinity induced by CaCl2, MgCl2, NaCl and Na2SO4 on the mobility of Cu, Cd, Pb and Zn was studied. An increase of ionic strength by any salts promoted a higher release of Cd than the others metals. When CaCl2 and NaCl were applied, Cd and Pb showed the highest degree of mobilization. When MgCl2 was applied, Cd and Cu were mobilized the most. Finally, an increase of Na2SO4 also promoted the strongest mobilization of Cd and Cu.As the total heavy metal content was higher, the percentage of Pb and Cu released upon salinization decreased, indicating that these metals are strongly bound to soil constituents. An increase of carbonates in the soil promoted a higher release of Pb for all used salts and for Zn when MgCl2 and NaCl were used. This indicates that Pb and Zn are adsorbed on the surface of carbonate crystals. An increase of fine particles promoted a decrease of percentage of released Cd for all salts, indicating that Cd is strongly retained in the fine fractions.The main mechanism regulating Pb and Cd mobility was competition with Ca2+ for sorption sites followed for metal chloro-complexation, association between the Cd/Pb-sulfates and competition with Mg2+. The main mechanism regulating Cu mobility was the formation of Cu-sulfate, followed by competition with cations (Mg > Ca) and chloride. For Zn, competition with Ca2+ for sorption sites was the most important process for its mobility; followed by Zn-sulfate association and, finally, chloride and competition with Mg with the same effect.  相似文献   

4.
An automatic process gas chromatograph has been developed for use on the recovery furnace stack of a Kraft pulp mill. The instrument analyzes for widely varying concentrations of H2S, SO2, CH3SH and higher order sulfur compounds. It is insensitive to the fixed gases and water vapor, and performs its analysis in approximately ten minutes. The instrument features a microcoulometric detector giving it sensitivity to H2S as low as 0.1 ppm, and SO2 and CH3SH as low as 0.5 ppm. The major limit to even higher sensitivity at this stage of development lies with two problems: the background noise level in the detector and the sulfur compound absorption in the Porapak Q chromatograph column. At the reported sensitivity, a 40-ml gas sample was used. The instrument also contains a data analysis system supplementary to the usual strip chart recorder. This system is made up of a digital voltmeter, a digital translator, and a teletype and hence allows the transfer of the output data to a digital computer for processing. The processed data are usually presented in the form of ppm quantities of the component gases in the stack gas. The instrument has worked successfully on small furnace effluent for periods of 25 hr but has not been tried on recovery furnace stacks. It has also run on prepared samples for periods of up to seven days with no maintenance or attendance necessary.  相似文献   

5.
ABSTRACT

As an odorless, nontoxic, and inert compound, sulfur hexafluoride (SF6) is one of the most widely used tracer gases in indoor air quality studies in both controlled and uncontrolled environments. This compound may be subject to reactions with water vapor under elevated temperature to form acidic inorganic compounds such as HF and H2SO4. Thus, in the presence of unvented combustion sources such as kerosene heaters, natural gas heaters, gas log fireplaces, candles, and lamps, the SF6 dissociation may interfere with measurements of the emissions from these sources. Tests were conducted in a research house with a vent-free natural gas heater to investigate these potential interferences. It was observed that the heater operation caused about a 5% reduction of SF6 concentration, which can be an error source for the ventilation rate measurement and consequently the estimated pollutant emission rates. Further analysis indicates that this error can be much greater than the observed 5% under certain test conditions because it is a function of the ventilation flow rate. Reducing the tracer gas concentration has no effect on this error. A simple theoretical model is proposed to estimate the magnitude of this error.

The second type of interference comes from the primary and secondary products of the SF6 dissociation, mainly H2SO4, SO2, HF, and fine particulate matter (PM). In the presence of ~5 ppm SF6, the total airborne concentrations of these species increased by a factor of 4-10. The tests were performed at relatively high SF6 concentrations, which is necessary to determine the interferences quantitatively. The second type of interference can be significantly reduced if the SF6 concentration is kept at a low ppb level.  相似文献   

6.
There is an appreciable chemical interaction between SO2 and photochemical smog which depends on the concentration of SO2 and water vapor. The rate of decay of SO2 concentration is greatly increased in the presence of photochemical smog. With 0.75 ppm SO2, a light-scattering aerosol is produced in dry systems and systems at 22 and 55% relative humidity (RH). Aerosol is not observed until after the NO2 peak has been reached and the NO concentration has fallen to a very low value. The formation of aerosol corresponds in time to the region of most rapid decrease in the SO2 profile. In systems at 65% RH or with smaller amounts of SO2, no light scattering is observed, but the percentage of SO2 disappearing is greater. In relatively dry systems the presence of SO2 results in a general slowing down of the photochemical smog reactions. In systems containing water vapor concentrations comparable to those found in the atmosphere, the inhibiting influence of SO2 on the smog reaction is less pronounced. However, the maximum concentration of oxidant produced by the photochemical smog reactions is significantly lower when SO2 is present.  相似文献   

7.
Results are presented as to the extent of chain scission (crosslinking) suffered by various polymers exposed to 1 atm of air and near ultraviolet light (λ > 2800 Å) in presence and absence of nitrogen dioxide, sulfur dioxide, and ozone, respectively, in the concentration range of 1 to 5 ppm. Vinyl polymers are scarcely affected by SO2 and NO2, respectively; however, nylon and elastomers are quite sensitive toward these gases. These conclusions agree with observations, found in the literature, on tensile tests, elongations, flexibilities, and infrared measurements in presence of sulfur dioxide under similar conditions.  相似文献   

8.
Abstract

Air pollutants were collected in Logan, Cache County, UT, in February 1993 during two periods of atmospheric inversion accompanied by fog. The following atmospheric species were determined: (1) gaseous SO2, NO2 (semi-quantitatively),HNO3, NH3, and HF; (2) fine particulate SO4 =, NO3 -, NH4 +, F–, H+, C, Si, S, K, Ca, Ti, Mn, Fe, Ni, Cu, Zn, Pb, Se, Br, and Sr, and; (3) fine particulate mass, which was calculated. The major components of fine particulate matter were carbonaceous material, ammonium nitrate, and ammonium sulfate, while the soil component was small. Calculated, fine particulate mass averaged 80 μg/m3 and reached concentrations as high as 120 μg/m3. SO2/Sox and NO2/NOy mole ratios generally varied between 0.2 and 0.1 during inversions. These ratios also showed moderate but consistent diurnal patterns. The emission inventory for Cache County indicates sources of SO2 and NOx but not significant amounts of primary sulfate and nitrate. The observations reported here indicate there is significant conversion of SO2 and NOx in the presence of excess oxidants to sulfuric and nitric acid that are neutralized by excess ammonia.  相似文献   

9.
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   

10.
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   

11.
The effects of the burning of fireworks on air quality in Beijing was firstly assessed from the ambient concentrations of various air pollutants (SO2, NO2, PM2.5, PM10 and chemical components in the particles) during the lantern festival in 2006. Eighteen ions, 20 elements, and black carbon were measured in PM2.5 and PM10, and the levels of organic carbon could be well estimated from the concentrations of dicarboxylic acids. Primary components of Ba, K, Sr, Cl, Pb, Mg and secondary components of C5H6O42−, C3H2O42−, C2O42−, C4H4O42−, SO42−, NO3 were over five times higher in the lantern days than in the normal days. The firework particles were acidic and of inorganic matter mostly with less amounts of secondary components. Primary aerosols from the burning of fireworks were mainly in the fine mode, while secondary formation of acidic anions mainly took place on the coarse particles. Nitrate was mainly formed through homogeneous gas-phase reactions of NO2, while sulfate was largely from heterogeneous catalytic transformations of SO2. Fe could catalyze the formation of nitrate through the reaction of α-Fe2O3 with HNO3, while in the formation of sulfate, Fe is not only the catalyst, but also the oxidant. A simple method using the concentration of potassium and a modified method using the ratio of Mg/Al have been developed to quantify the source contribution of fireworks. It was found that over 90% of the total mineral aerosol and 98% of Pb, 43% of total carbon, 28% of Zn, 8% of NO3, and 3% of SO42− in PM2.5 were from the emissions of fireworks on the lantern night.  相似文献   

12.
A sampling campaign of re-suspended road dust samples from 53 sites that could cover basically the entire Beijing, soil samples from the source regions of dust storm in August 2003, and aerosol samples from three representative sites in Beijing from December 2001 to September 2003, was carried out to investigate the characteristics of re-suspended road dust and its impact on the atmospheric environment. Ca, S, Cu, Zn, Ni, Pb, and Cd were far higher than its crustal abundances and Ca2+, SO42−, Cl, K+, Na+, NO3 were major ions in re-suspended road dust. Al, Ti, Sc, Co, and Mg in re-suspended road dust were mainly originated from crustal source, while Cu, Zn, Ni, and Pb were mainly derived from traffic emissions and coal burning, and Fe, Mn, and Cd were mainly from industrial emissions, coal combustion and oil burning. Ca2+ and SO42− mainly came from construction activities, construction materials and secondary gas-particle conversions, Cl and Na+ were derived from industrial wastewater disposal and chemical industrial emissions, and NO3 and K+ were from vehicle emissions, photochemical reactions of NOX, biomass and vegetable burning. The contribution of mineral aerosol from inside Beijing to the total mineral aerosols was ∼30% in spring of 2002, ∼70% in summer of 2002, ∼80% in autumn of 2003, ∼20% in PM10 and ∼50% in PM2.5, in winter of 2002. The pollution levels of the major pollution species, Ca, S, Cu, Zn, Ni, Pb, Fe, Mn, and Cd in re-suspended road dust reached ∼76%, ∼87%, ∼75%, ∼80%, ∼82%, ∼90%, ∼45%, ∼51%, and ∼94%, respectively. Re-suspended road dust from the traffic and construction activities was one of the major sources of pollution aerosols in Beijing.  相似文献   

13.
Abstract

This paper is particularly related to elemental mercury (Hg0) oxidation and divalent mercury (Hg2+) reduction under simulated flue gas conditions in the presence of nitric oxide (NO) and sulfur dioxide (SO2). As a powerful oxidant and chlorinating reagent, Cl2 has the potential for Hg oxidation. However, the detailed mechanism for the interactions, especially among chlorine (Cl)-containing species, SO2, NO, as well as H2O, remains ambiguous. Research described in this paper therefore focused on the impacts of SO2 and NO on Hg0 oxidation and Hg2+ reduction with the intent of unraveling unrecognized interactions among Cl species, SO2, and NO most importantly in the presence of H2O. The experimental results demonstrated that SO2 and NO had pronounced inhibitory effects on Hg0 oxidation at high temperatures when H2O was also present in the gas blend. Such a demonstration was further confirmed by the reduction of Hg2+ back into its elemental form. Data revealed that SO2 and NO were capable of promoting homogeneous reduction of Hg2+ to Hg0 with H2O being present. However, the above inhibition or promotion disappeared under homogeneous conditions when H2O was removed from the gas blend.  相似文献   

14.
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   

15.
Interest in air pollution injury to native vegetation has been generated with the construction and planned construction of large coal-fired power plants near the coal reserves in the southwest desert areas of the United States. Since information on the effects of SO2 on these native species was not available in the literature, fumigation studies were conducted with portable chambers placed over native species in the field with SO2 and SO2 + NO2. Pollutant concentrations were measured and controlled with instruments located in a mobile laboratory. Each fumigation was of two hours duration and the concentration ranged from 0.5 to 11 ppm SO2 and from 0.1 to 5 ppm NO2. Concentrations of SO2 above 2 ppm were required to cause injury to all but a few of the 87 species studied. Many of the native desert species proved to be highly resistant to injury from these gases.  相似文献   

16.
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   

17.
A new sampling device is described for the simultaneous collection of NH3, HNO3, HCl, SO2 and H2O2 in ambient air. The apparatus is based on air sampling by two parallel annular denuder tubes. The gases are collected by absorption in solutions present in the annulus of the denuder tubes. After a sampling time of 30 min at flow rate of 32 ℓ min−1 the solutions are extracted from the denuders and analyzed off-line. The detection limits of NH3, HNO3, HCL and SO2 are in the order of 0.1–0.5 μm−3. For H2O2 the detection limit is 0.01 μm−3. The reproducibility is 5–10% at the level of ambient air concentrations. Comparison of this novel technique with existing methods gives satisfactory results. The compact set-up offers the possibility of field experiments without the need of extensive equipment.  相似文献   

18.
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   

19.
In order to investigate the effects of humidity on the gas-phase oxidation of SO2 in polluted air and on the subsequent aerosol formation process, photoirradiation experiments were carried out by means of a 4-m3 chamber, in which mixtures containing SO2, NO and C3H6 with concentrations in the ppm range were exposed to simulated solar radiation in different relative humidity (r.h.) conditions. The total amount of oxidized SO2 was quantified from the SO42− yield determined by the chemical analysis of the aerosol product, and a part due to the oxidation by the OH radical was evaluated by estimating the OH concentration from the decay rate of C3H6. The remaining part was assigned to the oxidation by the Criegee intermediate, as it had a good correlation with the progress of the O3 + C3H6 reaction. The contributions of the two oxidizing species to the total conversion and the oxidation rate of SO2 were measured as functions of r.h. As a result, experimental evidence was obtained for the prediction of Calvert and Stockwell's (1983, Envir. Sci. Technol. 17, 428A–443A) simulation that the oxidation due to the Criegee intermediate was retarded by the increase in humidity. The OH contribution, on the other hand, was almost independent of r.h. It was observed consequently that the total oxidized amount of SO2 considerably decreased as r.h. was higher.The humidity effect on the aerosol formation process was found to be more complicated than the effect on the gas-phase chemistry. The maximum rate of increase in the particle number concentration rose linearly with increasing r.h., but the number concentration itself measured at its maximum or at the end of the irradiation reached a ceiling value around r.h. = 30% and went down for higher r.h. The average panicle size in the final stage of the reaction showed a minimum around the same r.h. at which the number concentration was maximum. The H2SO4 concentration in the mist particles, however, decreased monotonically as r.h. got higher. It was suggested that these different responses against the increase in humidity resulted from the cooperation of several processes such as the H2SO4 monomer formation, the H2O condensation, the particle coagulation, etc., which had different dependences on r.h.  相似文献   

20.
A laboratory study was conducted of the heterogeneous catalysis of sulfur dioxide at ppm concentrations in air by insoluble particles of CaCO2, V2O5, Fe203, flyash from a coal-burning power plant, MnCO2, activated carbon, and suspended particulate matter from urban air. The investigalion was performed by utilizing a new technique for aerosol stabilization which consists of depositing the aerosol on Teflon beads in a fluidized bed. The Teflon beads with deposited aerosol particles were then packed into a flow reactor. Progress of the chemical reaction of SO2 with deposited particles was continuously monitored by determining the SO2 concentrations in the reactor effluent with a microcoulometer.

In this investigation, CaCOg, V2O5, and flyash were essentially inert to SO2 at room temperature. Fe2O3, activated carbon, MnO2, and suspended particulate matter from urban air sorbed SO2 from air streams with up to 14.4 ppm SO2 in air. Evidence is presented which suggests that a substantial part of the sorbed SO2 was physically adsorbed.

Bioassay procedures which utilize pulmonary flow resistance changes in guinea pigs to monitor response to inhaled SO2-aerosol mixtures in air have indicated the weak or non-potentiating capacity of insoluble aerosols as contrasted to soluble aerosols. Potentiating response of an aerosol appears to be strongly associated with reaction of SO2 in a water droplet containing aerosol ions and not with physically adsorbed SO2 on an insoluble aerosol.  相似文献   

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