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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 following report discusses current bench- and pilot-plant advances in preparation of ADVAnced siliCATE (ADVACATE) calcium silicate sorbents for flue gas desulfurization. It also discusses current bench- and pilot-plant advances in sorbent preparation. Fly ash was ground in a laboratory scale grinder prior to slurring in order to decrease the slurring time needed for the sorbent to be reactive with SO2. Reactivity of ADVACATE sorbents with SO2 in the bench-scale reactor correlated with their surface area.

ADVACATE sorbents produced with ground fly ash were evaluated in the 50 cfm (85 m3/h) pilot plant providing 2 s duct residence time. ADVACATE sorbent was produced by slurrying ground fly ash (median particle size of 4.3 µm) with Ca(OH)2 at the weight ratio of 3:1 at 90°C (194°F) for 3hto yield solids with 30 weight percent of initial free moisture. When this sorbent was injected into the duct with 1500 ppm SO2 and at 11°C (20°F) approach to saturation, the measured SO2 removal was approximately 60percent at a Ca/S stoichiometric ratio of 2. Previously, when ADVACATE sorbent was produced at 90°C (194°F) and at the same fly-ash-to-Ca(OH)2 weight ratio using unground fly ash, removal under the same conditions in the duct was approximately 50 percent following 12 h slurring. The report presents the results of pilot-scale recycle tests at the recycle ratio of 2. Finally, the report discusses future U.S. Environmental Protection Agency plans for commercialization of ADVACATE.  相似文献   

3.
Pilot-scale tests were conducted to develop a combined nitrogen oxide (NOx) reduction technology using both selective catalytic reduction (SCR) and selective noncatalytic reduction (SNCR). A commercially available vanadium- and titanium-based composite honeycomb catalyst and enhanced urea (NH2CONH2) were used with a natural-gas-fired furnace at a NOx concentration of 110 ppm. Changes in SNCR chemical injection temperature and stoichiometry led to varying levels of post-furnace ammonia (NH3), which acts as the reductant feed to the downstream SCR catalyst. The urea-based chemical could routinely achieve SNCR plus SCR total NOx reductions of 85 percent with less than 3 ppm NH3 slip at reductant/NOx stoichiometries ranging from about 1.5 to 2.5 and SCR space velocities of 18,000 to 32,000 h?1. This pilot-scale research has shown that SNCR and SCR can be integrated to achieve high NOx removal. SNCR provides high temperature reduction of NOx followed by further removal of NOx and minimization of NH3 slip by a significantly downsized (high-space velocity) SCR.  相似文献   

4.
Abstract

Simultaneous removal of NH3 and H2S was investigated using two types of biofilters—one packed with wood chips and the other with granular activated carbon (GAC). Experimental tests and measurements included analyses of removal efficiency (RE), metabolic products, and results of long-term operation (around 240 days). The REs for NH3 and H2S were 92 and 99.9%, respectively, before deactivation. After deactivation, the RE for NH3 and H2S were decreased to 30–50% and 75%, respectively. The activity of nitrifying bacteria was inhibited by high concentrations of H2S (over 200 ppm) but recovered gradually after H2S addition was ceased. However, the Thiobacillus thioparus as sulfur oxidizing bacteria did not show inhibition at the NH3 concentration under 150-ppm conditions. The deactivation of the biofilter was caused by metabolic products [elemental sulfur and (NH4)2SO4] ac-cumulating on the packing materials during the extended operation. The removal capacities for NH3 and H2S were 6.0–8.0 and 45–75 mg N, S/L/hr, respectively.  相似文献   

5.
柱状V/AC催化剂的再生对脱硫活性的影响   总被引:1,自引:0,他引:1  
使用常压固定床反应器,考察了吸附SO2的柱状V/AC催化剂的热再生和NH3再生行为.结果表明:柱状V/AC催化剂再生过程中生成的SO2主要沿催化剂轴向由内部向外扩散.催化剂350 ℃NH3再生的效率高于热再生的效率.两次热再生后柱状V/AC催化剂的脱硫活性开始下降,而六次NH3再生后的脱硫活性仍保持不变,甚至还稍高于新鲜柱状V/AC催化剂的脱硫活性.柱状V/AC催化剂孔结构和元素分析结果表明,NH3再生使催化剂表面含N官能团增加,保护了催化剂小于1 nm的微孔.  相似文献   

6.
Previous workers have shown that simultaneous SO2/NOX removal can be obtained in a dry scrubbing system with Ca(OH)2 promoted by an additive such as NaOH, and that fly ash and product recycle improve the reactivity of the solids toward SO2. To test SO2/NOX removal with fly ash and product recycle, bench-scale experiments with a packed bed reactor were performed at bag filter conditions. The most reactive solid for NOX removal was prepared by slurrying Ca(OH)2 with fly ash, CaSO3, and NaOH. The best conditions for NOX removal were the greatest temperature (125°C) and greatest concentrations of SO2 (1500 ppm) and O2 (20 percent). At the best conditions, NOX removed in 1 hour was 3-4 moles per 100 moles Ca(OH)2, compared to 5-10 moles SO2 removed per 100 moles Ca(OH)2. The best SO2 removal was obtained at the highest relative humidities/lowest temperatures (55% RH/ 65°C) with solids prepared by slurrying Ca(OH)2 with fly ash and NaOH. At these conditions, SO2 removed In 1 hour was 60-80 moles per 100 moles Ca(OH)2, compared to 0.5 to 1 moles NOX removed per 100 moles Ca(OH)2.  相似文献   

7.
EPA’s efforts to develop low cost, retrofitable flue gas cleaning technology include the development of highly reactive sorbents. Recent work addressing lime enhancement and testing at the bench-scale followed by evaluation of the more promising sorbents in a pilot plant are discussed here.

The conversion of Ca(OH)2 with SO2 increased several-fold compared with Ca(OH)2 alone when Ca(OH)2 was slurrled with fly ash first and later exposed to SO2 in a laboratory packed bed reactor. Ca(OH)2 enhancement increased with the increased fly ash amount. Dlatomaceous earths were very effective reactivity promoters of lime-based sorbents. Differential scanning calorimetry of the promoted sorbents revealed the formation of a new phase (calcium silicate hydrates) after hydration, which may be the basis for the observed Improved SO2 capture.

Fly ash/lime and diatomaceous earth/lime sorbents were tested in a 100 m3/h pilot facility incorporating a gas humidifier, a sorbent duct injection system, and a baghouse. The inlet SO2 concentration range was 1000-2500 ppm. With once-through dry sorbent injection into the humidified flue gas [approach to saturation 10–20°C (18–36°F) in the baghouse], the total SO2 removal ranged from 50 to 90 percent for a stoichiometric ratio of 1 to 2. Recycling the collected solids resulted in a total lime utilization exceeding 80–90 percent. Increased lime utilization was also investigated by the use of additives.  相似文献   

8.
Caribbean pine, an economically important tree of tropical lowlands, is at risk of SO2 exposure in certain locales. Twenty-week old seedlings of Caribbean, Scots, and Virginia pine were exposed to 0.5, 1.0, and 2.0 ppm SO2 (1300, 2600, and 5200 μm?3, respectively) for 1, 2, 4, and 8 h in modified controlled-environment chambers. Severity of SO2-induced leaf necrosis for each species was related to SO2 concentration and exposure duration using a regression model. The three dose-response relationships differed in detail, but Caribbean pine seedlings were generally as sensitive to SO2 as seedlings of the two highly sensitive temperate species. In addition, 173 4-wk-old Caribbean pine seedlings were exposed to 0.5 ppm SO2 for 4 h. Over one-half of these seedlings exhibited some necrosis and over one-sixth had more than 5 percent of leaf surface necrotic. It is concluded that Caribbean pine seedlings are highly sensitive to acute doses of SO2.  相似文献   

9.
Incineration flue gas contains polycyclic aromatic hydrocarbons (PAHs) and sulfur dioxide (SO2). The effects of SO2 concentration (0, 350, 750, and 1000 ppm), reaction temperature (160, 200, and 280 °C), and the type of activated carbon fibers (ACFs) on the removal of SO2 and PAHs by ACFs were examined in this study. A fluidized bed incinerator was used to simulate practical incineration flue gas. It was found that the presence of SO2 in the incineration flue gas could drastically decrease removal of PAHs because of competitive adsorption. The effect of rise in the reaction temperature from 160 to 280 °C on removal of PAHs was greater than that on SO2 removal at an SO2 concentration of 750 ppm. Among the three ACFs studied, ACF-B, with the highest microporous volume, highest O content, and the tightest structure, was the best adsorbent for removing SO2 and PAHs when these gases coexisted in the incineration flue gas.
ImplicationsSimultaneous adsorption of sulfur dioxide (SO2) and polycyclic aromatic hydrocarbons (PAHs) emitted from incineration flue gas onto activated carbon fibers (ACFs) meant to devise a new technique showed that the presence of SO2 in the incineration flue gas leads to a drastic decrease in removal of PAHs because of competitive adsorption. Reaction temperature had a greater influence on PAHs removal than on SO2 removal. ACF-B, with the highest microporous volume, highest O content, and tightest structure among the three studied ACFs, was found to be the best adsorbent for removing SO2 and PAHs.  相似文献   

10.
In this study, we present ∼1 yr (October 1998–September 1999) of 12-hour mean ammonia (NH3), ammonium (NH4+), hydrochloric acid (HCl), chloride (Cl), nitrate (NO3), nitric acid (HNO3), nitrous acid (HONO), sulfate (SO42−), and sulfur dioxide (SO2) concentrations measured at an agricultural site in North Carolina's Coastal Plain region. Mean gas concentrations were 0.46, 1.21, 0.54, 5.55, and 4.15 μg m−3 for HCl, HNO3, HONO, NH3, and SO2, respectively. Mean aerosol concentrations were 1.44, 1.23, 0.08, and 3.37 μg m−3 for NH4+, NO3, Cl, and SO42−, respectively. Ammonia, NH4+, HNO3, and SO42− exhibit higher concentrations during the summer, while higher SO2 concentrations occur during winter. A meteorology-based multivariate regression model using temperature, wind speed, and wind direction explains 76% of the variation in 12-hour mean NH3 concentrations (n=601). Ammonia concentration increases exponentially with temperature, which explains the majority of variation (54%) in 12-hour mean NH3 concentrations. Dependence of NH3 concentration on wind direction suggests a local source influence. Ammonia accounts for >70% of NHx (NHx=NH3+NH4+) during all seasons. Ammonium nitrate and sulfate aerosol formation does not appear to be NH3 limited. Sulfate is primarily associated ammonium sulfate, rather than bisulfate, except during the winter when the ratio of NO3–NH4+ is ∼0.66. The annual average NO3–NH4+ ratio is ∼0.25.  相似文献   

11.
A year-long field study to characterize the ionic species in PM2.5 was carried out in Shanghai and Beijing, China, in 1999–2000. Weekly samples of PM2.5 were collected using a special low flow rate (0.4 l min−1) sampler. In Shanghai, SO42− NO3 and NH4+ were the dominant ionic species, which accounted for 46%, 18% and 17% of the total mass of ions, respectively. Local SO2 emissions were an important source of SO42− in PM2.5 because the SO42− concentration was correlated with the SO2 concentration (r=0.66). The relatively stable SO42−/SO2 mass ratio over a large range of temperatures suggests that gas-phase oxidation of SO2 played a minor role in the formation of SO42−. The sum of SO42− and NO3 was highly correlated with NH4+ (r=0.96), but insufficient ammonium was present to totally neutralize the aerosol. In Beijing, SO42−, NO3 and NH4+ were also the dominant ionic species, constituting 44%, 25% and 16% of the total mass of water-soluble ions, respectively. Local SO2 emissions were an important source of SO42− in the winter since SO42− was correlated with SO2 (r=0.83). The low-mass SO42−/SO2 ratio (0.27) during winter, which had low humidity, suggests that gas-phase oxidation of SO2 was a major route of sulfate formation. In the summer, however, much higher mass ratios of SO42−/SO2 (5.6) were observed and were ascribed to in-cloud sulfate formation. The annual average ratio of NO3/SO42− was 0.4 and 0.6 in Shanghai and in Beijing, respectively, suggesting that stationary emissions were still a dominant source in these two cities.  相似文献   

12.
ABSTRACT

Gaseous NH3 removal was studied in laboratory-scale biofilters (14-L reactor volume) containing perlite inoculated with a nitrifying enrichment culture. These biofilters received 6 L/min of airflow with inlet NH3 concentrations of 20 or 50 ppm, and removed more than 99.99% of the NH3 for the period of operation (101, 102 days). Comparison between an active reactor and an autoclaved control indicated that NH3 removal resulted from nitrification directly, as well as from enhanced absorption resulting from acidity produced by nitrification. Spatial distribution studies (20 ppm only) after 8 days of operation showed that nearly 95% of the NH3 could be accounted for in the lower 25% of the biofilter matrix, proximate to the port of entry. Periodic analysis of the biofilter material (20 and 50 ppm) showed accumulation of the nitrification product NO3 - early in the operation, but later both NO2 - and NO3 - accumulated. Additionally, the N-mass balance accountability dropped from near 100% early in the experiments to ~95 and 75% for the 20- and 50-ppm biofilters, respectively. A partial contributing factor to this drop in mass balance accountability was the production of NO and N2O, which were detected in the biofilter exhaust.  相似文献   

13.
The characteristics of water-soluble inorganic ions (WSIIs) during a winter period in a suburb of Xi'an, China, were investigated. Our results show that the total mass concentration of the dominant WSIIs (8) was 91.27 µg m–3, accounting for 50.1% of the total mass concentration of PM2.5 (particulates with a size of 2.5 µm or less). Secondary inorganic aerosols (SO42?, NO3? and NH4+) were the most abundant ions, accounting for up to 95.12% of the total ions. By using the anion and cation equivalence ratio method, PM2.5 was shown to have weak alkalinity, and the chemical forms of WSIIs were mainly (NH4)2SO4 and NH4NO3. The sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR) suggested that larger proportions of SO42? and NO3? were formed by gas-phase SO2 and NO2 in the sampling site. Ratio analysis also indicated that anthropogenic sources significantly contributed to WSII pollution. Among the anthropogenic sources, fixed pollution sources were found to be dominant over mobile sources.  相似文献   

14.
Abstract

Annual applications of (NH4)2SO4 NH4NO3 and urea on a Solonetzic soil at 112 kg N/ha for 10 consecutive years reduced pH levels from 5.6 for the check to 4.4, 4.9 and 5.3, respectively for (NH4)2SO4, NH4NO3 and urea. (NH4)2SO4 generated twice as much exchange acidity as NH4NO3 and four times as much as urea. Net extractable cations leached from the Ap horizon closely approximated the amount of exchange acidity generated by (NH4)2SO4 and NH4NO3 fertilizers. The levels of soil extractable Al and Mn were greatly enhanced by (NH4)2SO4 as were plant contents. Similar acidifying effects to that produced by the (NH4)2SO4 occurred when NH4NO3 was applied at 300 kg N/ha annually for 12 consecutive years in another field experiment on the same soil. Liming samples of the field (NH4)2SO4 acidified soils in the greenhouse, significantly increased yields and lowered the Al and Mn contents of the plants to normal levels.  相似文献   

15.
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   

16.
采用移动床生物膜反应器(MBBR)处理配制模拟废水,实验结果表明,水力停留时间为6h、悬浮填料填充率为40%时,在不同C/N/P比率条件下,MBBR对COD、NH4+-N和TN去除性能好且稳定,平均去除率分别达到90%、94.8%和62.39%以上,而TP的去除率受C/N/P值影响较大,当C/N/P的比值为100/10/1.8时,平均去除率达到58.03%。一定的溶解氧(DO)质量浓度能保证反应器中COD、NH4-N高效稳定的去除,同时是TN和TP同时去除的重要影响因素,在MBBR中最佳DO值约为3mg/L。由于附着在悬浮填料生物膜内部存在厌氧、缺氧微环境条件,在反应器中存在少量的反硝化聚磷菌。  相似文献   

17.
A series of experiments using bulk precipitation collectors of the type used in the UK precipitation chemistry network measured the amounts of NH4+, SO42− and other ions that could be washed from funnels (diameter 15 cm) exposed to a wide range of NH3 and SO2 concentrations over periods from hours to days. In dry conditions, the average deposition flux of NH3 was between 50 and 120 nmol NH4+ funnel−1 d−1 (0.1–0.3 kg N ha−1 yr−1), and was independent of the concentration of NH3. Dry deposition of NH3 to wet funnels at small NH3 concentrations was almost 5 times that to dry funnels under the same conditions (average 240 nmol funnel−1 d−1; 0.7 kg ha−1 yr−1), and increased with increasing NH3 concentrations. The amount of NH4+ ions remaining on the funnel surface was inversely proportional to the vapour pressure deficit during the experiment. This result was interpreted as a dependence on the duration of surface wetness, with greater deposition of NH4+ when evaporation rates of surface water were small.The amount of SO2 deposited on funnel surfaces was closely related to the amount of NH3 deposited, in both wet and dry conditions, but was not strongly correlated with the SO2 concentration. At low NH3 and SO2 concentrations the average deposition to dry funnels was 70 nmol SO42− funnel−1 d−1 (0.5 kg ha−1 yr−1), and to wet funnels was approximately 2.5 times larger. The results are interpreted in terms of the balance between the rate of evaporation of surface water, and the rate of oxidation of SO2, which leads to the ‘fixing’ of NH4+ ions on the surface as involatile salts.It is predicted that dry deposition of NH3 to funnel surfaces across the UK Secondary Network could account for as much as one-half of the measured bulk wet deposition at sites where wet deposition of NH4–N is small. The amount of dry deposition depends on how long and how often funnel surfaces are wetted by rain or dew, and on the air concentrations of NH3. These predictions are based on funnels being wetted only once per day. More frequent wetting would increase the contribution from dry deposition, and the consequent overestimate of wet deposition of NH4–N across the UK by using data obtained from bulk collectors. To some extent this overestimate may be offset by microbial degradation and loss of NH4–N in weekly bulk precipitation samples during collection and storage.  相似文献   

18.
采用2套启动成功的上向流厌氧氨氧化(ANAMMOX)生物滤柱,通过调节进水NaNO2和(NH42SO4 的浓度负荷及水力负荷,改变进水容积负荷,探讨容积负荷对ANAMMOX生物滤柱脱氮效能的影响及其动力学模型。结果表明,滤速恒定条件下,通过提高进水基质浓度来提高进水TN容积负荷,其容积负荷去除动力学过程符合Monod-Haldane基质抑制模型。进水NH4+-N与NO2--N浓度分别低于100 mg/L和133 mg/L时,反应器脱氮效果不受明显影响,TN容积去除负荷可达4.21 kg/(m3·d),TN去除率可达80%以上。进水基质浓度恒定条件下,通过提高滤速来提高进水TN容积负荷,其容积负荷去除动力学过程符合零级动力学方程。不受基质浓度抑制的条件下,滤速为3.0 m/h、进水容积负荷为8.82 kg/(m3·d)时,反应器总氮容积负荷去除量可达7.15 kg/(m3·d),总氮去除率可达81.1%。  相似文献   

19.
Novel silica-enhanced lime sorbents were tested in a bench-scale sand-bed reactor for their potential for SO2 removal from flue gas. Reactor conditions were 64°C (147°F), relative humidity of 60 percent [corresponding to an approach to saturation temperature of 10°C (18°F)], and inlet SO2 concentration of 500 or 1000 ppm. The sorbents were prepared by pressure hydration of CaO or Ca(OH)2 with siliceous materials at 100°C (101 kPa) [212°F (14.7 psi)] to 230°C (2793 kPa) [446°F (405 psi)] for 15 min to 4 h. Pressure hydration fostered the formation of a sorbent reactive with SO2 from fly ash and Ca(OH)2 in a much shorter time than did atmospheric hydration. The conversion of Ca(OH)2 in the sand-bed reactor increased with the increasing weight ratio of fly ash to lime and correlated well with B.E.T. surface area, increasing with increasing surface area. The optimum temperature range for the pressure-hydration of fly ash with Ca(OH)2 was between 110 and 160°C (230 and 320 °F). The pressure hydration of diatomaceous earth with CaO did not offer significant reactivity advantages over atmospheric hydration; however, the rate of enhancement of Ca(OH)2 conversions was much faster with pressure hydration. Scanning electron microscope (SEM) and x-ray diffraction studies showed solids of different morphology with different fly ash/lime ratios and changing conditions of pressure hydration.  相似文献   

20.
As a part of a receptor model study of the Philadelphia, PA atmosphere, particulate samples were collected from seven air pollution sources in the area: two oil-fired power plants, a coal-fired power plant, a fluidized catalytic cracker, a refuse incinerator, a secondary aluminum smelter and an antimony ore roaster. Samples were collected In two size fractions with a dilution source sampler connected to a modified dichotomous sampler. Masses of collected material were determined gravlmetrlcally. Samples were analyzed for elements by x-ray fluorescence followed by Instrumental neutron activation analysis of some samples. Other samples were analyzed by chemical methods for volatile and nonvolatile carbon, SO4 2? and NH4 +. Data are presented for up to 46 elements and species on fine (<2.5-μm aerodynamic equivalent diameter) and coarse (2.5 μm < diam < 7-10 μm) particles from each source. Although the data were collected for use in Philadelphia, they should be of value for receptor modeling of other areas having similar sources. The most unexpected results were the large amounts of rare earth elements on particles from the catalytic cracker (e.g., 0.31 percent La In fine fraction) and the oil-fired power plants (120 and 420 ppm La in fine fraction). Substantial amounts of primary SO4 2? are released from the oil-fired plants, the SO4 2? concentrations accounting for 40-45 percent of the fine particulate mass.  相似文献   

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