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1.
以锐钛矿型二氧化钛和钛钨粉(5%WO3-TiO2)为载体,制备了系列钒和钨负载量不同的钒钛催化剂,考察碱金属和碱土金属(钾、钠和钙)对催化剂在氨选择性催化还原(NH3-SCR)氮氧化物反应中催化活性的影响。钾、钠和钙对钒钛催化剂的中毒影响大小顺序为钾钠钙。提高钒钛催化剂中钒的含量可显著提高催化剂的SCR活性和抗碱金属中毒性能,但高钒负载量(4.5%V2O5)造成催化剂氮气选择性明显下降,氧化亚氮生成显著增加。钨的添加有利于提高钒钛催化剂的低温活性和抗碱金属中毒性能,对氮气选择性无明显影响。  相似文献   

2.
Abstract

A study was conducted to investigate the effect of selective catalytic reduction (SCR) catalyst on mercury (Hg) speciation in bituminous and subbituminous coal combustion flue gases. Three different Illinois Basin bituminous coals (from high to low sulfur [S] and chlorine [Cl]) and one Powder River Basin (PRB) subbituminous coal with very low S and very low Cl were tested in a pilot-scale combustor equipped with an SCR reactor for controlling nitrogen oxides (NOx) emissions. The SCR catalyst induced high oxidation of elemental Hg (Hg0), decreasing the percentage of Hg0 at the outlet of the SCR to values <12% for the three Illinois coal tests. The PRB coal test indicated a low oxidation of Hg0 by the SCR catalyst, with the percentage of Hg0 decreasing from ~96% at the inlet of the reactor to ~80% at the outlet. The low Cl content of the PRB coal and corresponding low level of available flue gas Cl species were believed to be responsible for low SCR Hg oxidation for this coal type. The test results indicated a strong effect of coal type on the extent of Hg oxidation.  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

This study investigated the effect of adding vanadium (V) to natural manganese oxide (NMO) in ammonia (NH3) selective catalytic reduction (SCR). The addition of V to NMO decreased the catalytic activity at low temperatures by blocking the active site. However, the enhancement of catalytic activity was achieved by controlling NH3 oxidation at high temperatures. From the NH3 temperature programmed desorption and oxygen on/off test, it was confirmed that the amount of Lewis acid site and active lattice oxygen of the catalyst affects the catalytic performance at low temperature

IMPLICATIONS Recently, NMO and manganese oxide have been reported as SCR catalysts. They usually have only reported the reaction characteristics and catalytic activity on the NH3 SCR over NMO or manganese/metal oxide catalysts. There are no studies about the effect of addition of V to NMO. Therefore, this study investigates the catalytic activity and reaction characteristics on the NH3 SCR over NMO and V/NMO, and a new application is proposed based on the conclusions of this study.  相似文献   

5.
A series of manganese-cerium oxide (MnOx-CeO2) catalysts supported by Ti-bearing blast furnace slag were prepared by wet impregnation and used for low-temperature selective catalytic reduction (SCR) of NO with NH3. The slag-based catalyst exhibited high nitrogen oxide removal (deNOx) activity and wide effective temperature range. Under the condition of NO = 500 ppm, NH3 = 500 ppm, O2 = 7–8 vol%, and total flow rate = 1600 mL/min, the Mn-Ce/Slag catalyst exhibited a NO conversion higher than 95% in the range of 180–260 °C. The activity of Mn/Slag catalysts was greatly enhanced with the addition of CeO2. The results indicated that Ti-bearing blast furnace slag had suitable phase composition as good support of SCR catalyst.

Implications: Ti-bearing blast furnace slag is a kind of industrial waste in China. Much slag was underused and piling up, which could cause many environmental issues, such as enormous waste of titanium and groundwater and soil contamination by heavy metals in leachates. The utilization of slag as the support of SCR catalyst will not only make use of solid waste but also cut down the NOx emitted from power plant.  相似文献   


6.
A hybrid selective noncatalytic reduction/selective catalytic reduction (SNCR/SCR) system that uses two types of technology, low-temperature SCR process and SNCR process, was designed to develop nitrogen oxide (NOx) reduction technology. SCR was conducted with space velocity (SV) = 2400 hr?1 and hybrid SNCR/SCR with SV = 6000 hr?1, since the study focused on reducing the amount of catalyst and both achieved 98% NOx reduction efficiency. Characteristics of NOx reduction by NH3 were studied for low-temperature SCR system at 150 °C using Mn-V2O5/TiO2 catalyst. Mn-added V2O5/TiO2 catalyst was produced, and selective catalyst reduction of NOx by NH3 was experimented. NOx reduction rate according to added Mn content in Mn-V2O5/TiO2 catalyst was studied with varying conditions of reaction temperature, normalized stoichiometric ratio (NSR), SV, and O2 concentration. In the catalyst experiment according to V2O5 concentration, 1 wt.% V2O5 catalyst showed the highest NOx reduction rate: 98% reduction at temperature window of 200~250 °C. As a promoter of the V2O5 catalyst, 5 wt.% Mn was added, and the catalyst showed 47~90% higher efficiency even with low temperatures, 100~200 °C. Mn-V2O5/TiO2 catalyst, prepared by adding 5 wt.% Mn in V2O5/TiO2 catalyst, showed increments of catalyst activation at 150 °C as well as NOx reduction. Mn-V2O5/TiO2 catalyst showed 8% higher rate for NOx reduction compared with V2O5/TiO2 catalyst in 150 °C SCR. Thus, (5 wt.%)Mn-(1 wt.%)V2O5/TiO2 catalyst was applied in SCR of hybrid SNCR/SCR system of low temperature at 150 °C. Low-temperature SCR hybrid SNCR/SCR (150 °C) system and hybrid SNCR/SCR (350 °C) showed 91~95% total reduction rate with conditions of SV = 2400~6000 hr?1 SCR and 850~1050 °C SNCR, NSR = 1.5~2.0, and 5% O2. Hybrid SNCR/SCR (150 °C) system proved to be more effective than the hybrid SNCR/SCR (350 °C) system at low temperature.

Implications:?NOx control is very important, since they are the part of greenhouse gases as well as the cause of acid rain and ozone hole. A technology, so-called hybrid SNCR/SCR process, was tested using Mn-V2O5/TiO2 monolithic catalyst for NOx reduction, and the method is promising. The results of this study would provide some ideas to parties such as policy makers, environmental engineers, and so on.  相似文献   

7.
A series of iron–manganese oxide catalysts supported on TiO2 and titanium nanotubes (TNTs) were studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in the presence of SO2. The results showed that the specific surface area and the amount of Brønsted acid sites were highly correlated. The results also demonstrated that higher Mn4+/Mn3+ ratios and larger specific surface areas might be the main reasons for the excellent performance of MnFe-TNTs catalyst after SO2 poisoning. The SO2 poisoning effect could be minimized by reducing the GHSV, increasing the reaction temperature, or increasing the [NH3]/[NO] molar ratio. The results also indicated that the formation of ammonium sulfate had a stronger effect on the NO conversion efficiency as compared to the formation of metal sulfate. Thus operating the low temperature SCR at above 230 oC to avoid the formation of ammonium sulfate would be the priority choice when SO2 poisoning is a concerned issue.?Implications: Low-temperature selective catalytic reduction (SCR) has attracted increasing attention due to that it can reduce the energy consumption for the SCR process employed in industries such as steel plants and glass manufacturing plants. However, it also suffers from the sulfur dioxide (SO2) poisoning problem. This study investigates the possibility of using titania nanotubes (TNTs) as the support of Mn/Fe bimetal oxide catalysts for low-temperature SCR to reduce the SO2 poisoning. The results indicated that the MnFe-TNT catalyst can tolerate SO2 for a longer time as compared with the MnFe-TiO2 catalyst.  相似文献   

8.
In this study, the authors investigated the influence of the valence state of Mn on the efficacy of selective catalytic reduction using a Mn-based catalyst. The nitrogen oxides (NOx) conversion rate of the catalyst was found to be dependent on the type of TiO2 support employed and on the temperature, as the catalyst showed an excellent conversion of > 80% at a space velocity of 60,000 hr?1 when the temperature was above 200 °C. Brunauer-Emmett-Teller, X-ray diffraction, and X-ray photoelectron spectroscopy analyses confirmed that catalyst displaying the highest activity contained the Mn4+ species and that its valence state was highly dependent on the pH during the catalyst preparation.
Implications Recently, various Mn catalysts have been evaluated as selective catalyst reduction (SCR) catalysts. However, in these previous studies, only the reaction characteristics and catalytic activity on the NH3 SCR over Mn catalysts were evaluated. There have been no studies on the effect of pH during catalyst preparation. Therefore, in this study, the effect of pH during the catalyst preparation process was examined and a new application of the Mn catalysts was proposed based on the current findings.  相似文献   

9.
低温选择性催化还原(SCR)脱硝是国内外脱硝技术研发的热点,但目前主要集中在实验室小试范围,无法完全反映催化剂在实际烟气中的运行状况。在30 t/h循环流化床燃煤锅炉脱硫除尘装置后建设了2 000~5 000 m3/h的SCR脱硝中试装置,经系统研究发现,中试使用的蜂窝式催化剂对SO2和NO具有很强的吸附能力,且反应温度、喷氨速率和气体空速均会影响催化脱硝效率。为期5 d的连续运行实验结果表明,催化剂的脱硝效率一直稳定在30%~50%,并未发现明显的失活,这证明设计除雾除尘器、较大的混合器、混合器与反应器间较长的管路均有利于缓解催化剂因SO2、H2O和飞灰中的碱性金属导致的失活。  相似文献   

10.
A study was conducted to investigate the effect of selective catalytic reduction (SCR) catalyst on mercury (Hg) speciation in bituminous and subbituminous coal combustion flue gases. Three different Illinois Basin bituminous coals (from high to low sulfur [S] and chlorine [Cl]) and one Powder River Basin (PRB) subbituminous coal with very low S and very low Cl were tested in a pilot-scale combustor equipped with an SCR reactor for controlling nitrogen oxides (NOx) emissions. The SCR catalyst induced high oxidation of elemental Hg (Hg0), decreasing the percentage of Hg0 at the outlet of the SCR to values <12% for the three Illinois coal tests. The PRB coal test indicated a low oxidation of Hg0 by the SCR catalyst, with the percentage of Hg0 decreasing from approximately 96% at the inlet of the reactor to approximately 80% at the outlet. The low Cl content of the PRB coal and corresponding low level of available flue gas Cl species were believed to be responsible for low SCR Hg oxidation for this coal type. The test results indicated a strong effect of coal type on the extent of Hg oxidation.  相似文献   

11.
Abstract

This paper introduces a predictive mechanism for elemental mercury (Hg0) oxidation on selective catalytic reduction (SCR) catalysts in coal-fired utility gas cleaning systems, given the ammonia (NH3)/nitric oxide (NO) ratio and concentrations of Hg0 and HCl at the monolith inlet, the monolith pitch and channel shape, and the SCR temperature and space velocity. A simple premise connects the established mechanism for catalytic NO reduction to the Hg0 oxidation behavior on SCRs: that hydrochloric acid (HCl) competes for surface sites with NH3 and that Hg0 contacts these chlorinated sites either from the gas phase or as a weakly adsorbed species. This mechanism explicitly accounts for the inhibition of Hg0 oxidation by NH3, so that the monolith sustains two chemically distinct regions. In the inlet region, strong NH3 adsorption minimizes the coverage of chlorinated surface sites, so NO reduction inhibits Hg0 oxidation. But once NH3 has been consumed, the Hg0 oxidation rate rapidly accelerates, even while the HCl concentration in the gas phase is uniform. Factors that shorten the length of the NO reduction region, such as smaller channel pitches and converting from square to circular channels, and factors that enhance surface chlorination, such as higher inlet HCl concentrations and lower NH3/NO ratios, promote Hg0 oxidation.

This mechanism accurately interprets the reported tendencies for greater extents of Hg0 oxidation on honeycomb monoliths with smaller channel pitches and hotter temperatures and the tendency for lower extents of Hg0 oxidation for hotter temperatures on plate monoliths. The mechanism also depicts the inhibition of Hg0 oxidation by NH3 for NH3/NO ratios from zero to 0.9. Perhaps most important for practical applications, the mechanism reproduces the reported extents of Hg0 oxidation on a single catalyst for four coals that generated HCl concentrations from 8 to 241 ppm, which covers the entire range encountered in the U.S. utility industry. Similar performance is also demonstrated for full-scale SCRs with diverse coal types and operating conditions.  相似文献   

12.
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   

13.
The deposition velocity of NH3 on six plant species at environmental concentrations has been studied in a dynamic plant gas exchange reactor. The total resistance to the transport of NH3 was studied. The aerodynamic resistance was determined directly by NH3 gas absorption in aqueous solutions at environmental concentrations in a two-phase gradientless reactor modeling the transfer processes through the stomata in a leaf. The concentration of NH3 in the gas phase ranged from 50 to 1000 ppb and the temperature varied from 25 to 30°C. The results for the deposition velocity for NH3, during the day, varied from 0.3 to 1.3 cm/s. The deposition velocities at night were about one order of magnitude smaller. These results are compared with estimates from the Frdssling equation which consistently yields higher values of the same order of magnitude. To determine accurate atmospheric transport models or global budget models, a variable deposition velocity should be used to account for the diurnal and seasonal variations in the surface resistance.  相似文献   

14.
A bench-scale reactor consisting of a natural gas burner and an electrically heated reactor housing a selective catalytic reduction (SCR) catalyst was constructed for studying elemental mercury (Hg(o)) oxidation under SCR conditions. A low sulfur Powder River Basin (PRB) subbituminous coal combustion fly ash was injected into the entrained-flow reactor along with sulfur dioxide (SO2), nitrogen oxides (NOx), hydrogen chloride (HCl), and trace Hg(o). Concentrations of Hg(o) and total mercury (Hg) upstream and downstream of the SCR catalyst were measured using a Hg monitor. The effects of HCl concentration, SCR operating temperature, catalyst space velocity, and feed rate of PRB fly ash on Hg(o) oxidation were evaluated. It was observed that HCl provides the source of chlorine for Hg(o) oxidation under simulated PRB coal-fired SCR conditions. The decrease in Hg mass balance closure across the catalyst with decreasing HCl concentration suggests that transient Hg capture on the SCR catalyst occurred during the short test exposure periods and that the outlet speciation observed may not be representative of steady-state operation at longer exposure times. Increasing the space velocity and operating temperature of the SCR led to less Hg(o) oxidized. Introduction of PRB coal fly ash resulted in slightly decreased outlet oxidized mercury (Hg2+) as a percentage of total inlet Hg and correspondingly resulted in an incremental increase in Hg capture. The injection of ammonia (NH3) for NOx reduction by SCR was found to have a strong effect to decrease Hg oxidation. The observations suggest that Hg(o) oxidation may occur near the exit region of commercial SCR reactors. Passage of flue gas through SCR systems without NH3 injection, such as during the low-ozone season, may also impact Hg speciation and capture in the flue gas.  相似文献   

15.
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   

16.
Emission factors for elemental metals were determined from several heavy-duty diesel vehicles (HDDV) of 1998–2007 vintage, operating with advanced PM and/or NOX emissions control retrofits on a heavy-duty chassis dynamometer, under steady state cruise, transient, and idle conditions. The emission control retrofits included diesel particulate filters (DPF): catalyzed and uncatalyzed, passive and active prototype vanadium- or zeolite-based selective catalytic reduction (SCR) systems, and a catalyzed DPF fitted on a hybrid diesel electric drive vehicle. The prototype SCR systems in combination with DPF retrofits are of particular interest because they represent the expected emissions controls for compliance with PM and NOX regulations in 2010. PM samples from a full-exhaust dilution tunnel were collected on bulk filters, and on a Personal Cascade Impactor Sampler (PCIS) for total and water-soluble elemental analysis. All the DPFs significantly reduced emissions of total trace elements (>85% and >95% for cruise and for the Urban Dynamometer Driving Schedule (UDDS), respectively). However, we observed differences in the post-retrofit metals emissions due to driving cycle effects (i.e., exhaust temperature) and type of retrofit. In general, the metals emissions over cruise conditions (which leads to higher exhaust temperatures) were substantially different from the emissions over a transient cycle or while idling. For instance, during cruise, we observed higher levels of platinum (1.1 ± 0.6–4.2 ± 3.6 ng km?1) for most of the retrofit-equipped vehicle tests compared to the baseline configuration (0.3 ± 0.1 ng km?1). The vanadium-based DPF + SCR vehicle during cruise operation exhibited emissions of vanadium (562 ± 265 ng km?1) and titanium (5841 ± 3050 ng km?1), suggesting the possible release of actual SCR wash-coat (V2O5/TiO2) from the catalyst under the higher temperatures characteristic of cruise operation. The vanadium emissions exhibited a bi-modal mass size distribution, with modes at <0.25 μm and 1.0–2.5 μm size ranges for the vanadium-based SCR system. For the DPF + SCR systems, a greater fraction of the metal emissions from the zeolite-based system is water-soluble compared to emissions from the vanadium-based system.  相似文献   

17.
在人工配制的污水中投入一定量的基质,不同条件下振荡培养,评价沸石、炉渣和陶瓷滤料3种基质在不同因素影响下对氨氮(NH4+-N)和总磷(TP)的吸附能力。结果表明,不同吸附时间时,沸石对NH4+-N的吸附效果最好,陶瓷滤料对TP的吸附效果最好;进水浓度对沸石吸附NH4+-N的影响较大,其吸附量随进水浓度的增大而增大,进水浓度对炉渣和陶瓷滤料吸附NH4+-N及炉渣吸附TP影响不大;3种基质对NH4+-N和TP的吸附量均是随吸附剂量的增加而降低,要达到较好的去污效果,应根据实验结果考虑基质投入量;pH值对沸石吸附NH4+-N影响显著,pH值6~7范围内吸附效果最好,pH值8~12的碱性条件有利于基质对TP的吸附。  相似文献   

18.
Abstract

The speciation of Hg in coal-fired flue gas can be important in determining the ultimate Hg emissions as well as potential control options for the utility. The effects of NOx control processes, such as selective catalytic reduction (SCR) and selective non-catalytic reduction (SNCR), on Hg speciation are not well understood but may impact emissions of Hg. EPRI has investigated the reactions of Hg in flue gas at conditions expected for some NOx control processes. This paper describes the methodology used to investigate these reactions in actual flue gas at several power plants. Results have indicated that some commercial SCR catalysts are capable of oxidizing elemental Hg in flue gas obtained from the inlets of SCR or air heater units. Results are affected by various flue gas and operating parameters. The effect of flue gas composition, including the presence of NH3, has been evaluated. The influence of NH3 on fly ash Hg reactions also is being investigated.  相似文献   

19.
Measurements on size distribution of atmospheric aerosol were made at Dayalbagh, Agra during July to September 1998. A 4-stage cascade particle sampler (CPS - 105) which fractionates particles in sizes ranging between 0.7 and >10.9 μm, was used. Samples were collected on Whatman 41 filters. The filters were analyzed for the major water-soluble ions. The anions (F, Cl, NO3 and SO4) were analyzed by Dionex DX-500 ion chromatograph while atomic absorption and colorimetric techniques were used for the analysis of cations (Na, K, Ca and Mg) and NH4, respectively. The average mass of aerosol was found to be 131.6 μg m−3 and aerosol composition was found to be influenced by terrigeneous sources. The mass size distribution of total aerosol and the ions NH4, Cl, NO3, K, Ca, Mg, SO4 and Na was bimodal while that of F was unimodal. SO4, F, K and NH4 dominated in the fine mode while Ca, Mg, Cl and NO3 were in abundance in coarse fraction. Na was found in both coarse as well as fine mode. Coarse mode SO4 and NO3 have been ascribed to contribution from re-suspension of soil and formation by heterogeneous oxidation on soil derived particles. Preponderance of K in fine mode is attributed to emissions from vegetation and from burning of plant materials. Ca, Mg, Cl and NO3 are largely soil derived and hence dominate in coarse fraction. Equivalent ratios of NH4/(SO4+NO3) were calculated for both fine and coarse aerosols. The coarse mode ratio varied between 0.7 and 1.4 while in fine mode it ranged between 1.4 and 1.9. It shows that aerosol is basic, the basicity of coarse mode is due to higher concentration of soil-derived alkaline components while the basicity in fine mode is due to neutralization of acidity by NH3.  相似文献   

20.
氧化锰矿渣改性制备SCR脱硝催化剂   总被引:2,自引:1,他引:1  
以锰酸钾生产过程中产生的氧化锰矿渣为原料,制备了一系列Mn基SCR脱硝催化剂。研究了活性炭、二氧化钛、以及含锰量的变化对催化剂的脱硝活性的影响。结果表明,直接由矿渣制备的催化剂和添加活性炭、二氧化钛制备的催化剂,其最大脱硝率分别为40%和78%。XPS表征发现催化剂中的锰元素存在多种氧化价态,活性炭的加入在一定程度上改变了不同价态之间的相对含量;在矿渣中加入硫酸锰后,发现总锰含量达到10%时,催化剂的最大脱硝率从78%降低至57%,XRD测试发现硫酸锰的加入导致S2O27-物种的生成,可能是引起催化剂活性下降的原因之一;而加入醋酸锰至总锰含量达到10%时,增大了催化剂的活性温度窗口,当总锰含量达到20%时,在空速10 000 h-1条件下,催化剂的最大脱硝率达到86.7%。  相似文献   

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