首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 640 毫秒
1.
Fe2O3 and CeO2 modified activated coke (AC) synthesized by the equivalent-volume impregnation were employed to remove elemental mercury (Hg0) from simulated flue gas at a low temperature. Effects of the mass ratio of Fe2O3 and CeO2, reaction temperature, and individual flue gas components including O2, NO, SO2, and H2O (g) on Hg0 removal efficiency of impregnated AC were investigated. The samples were characterized by Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). Results showed that with optimal mass percentage of 3 % Fe2O3 and 3 % CeO2 on Fe3Ce3/AC, the Hg0 removal efficiency could reach an average of 88.29 % at 110 °C. Besides, it was observed that O2 and NO exhibited a promotional effect on Hg0 removal, H2O (g) exerted a suppressive effect, and SO2 showed an insignificant inhibition without O2 to some extent. The analysis of XPS indicated that the main species of mercury on used Fe3Ce3/AC was HgO, which implied that adsorption and catalytic oxidation were both included in Hg0 removal. Furthermore, the lattice oxygen, chemisorbed oxygen, and/or weakly bonded oxygen species made a contribution to Hg0 oxidation.  相似文献   

2.
Abstract

Selective catalytic reduction (SCR) technology increasingly is being applied for controlling emissions of nitrogen oxides (NOx) from coal-fired boilers. Some recent field and pilot studies suggest that the operation of SCR could affect the chemical form of mercury (Hg) in coal combustion flue gases. The speciation of Hg is an important factor influencing the control and environmental fate of Hg emissions from coal combustion. The vanadium and titanium oxides, used commonly in the vanadia-titania SCR catalyst for catalytic NOx reduction, promote the formation of oxidized mercury (Hg2+).

The work reported in this paper focuses on the impact of SCR on elemental mercury (Hg0) oxidation. Bench-scale experiments were conducted to investigate Hg0 oxidation in the presence of simulated coal combustion flue gases and under SCR reaction conditions. Flue gas mixtures with different concentrations of hydrogen chloride (HCl) and sulfur dioxide (SO2) for simulating the combustion of bituminous coals and subbituminous coals were tested in these experiments. The effects of HCl and SO2 in the flue gases on Hg0 oxidation under SCR reaction conditions were studied. It was observed that HCl is the most critical flue gas component that causes conversion of Hg0 to Hg2+ under SCR reaction conditions. The importance of HCl for Hg0 oxidation found in the present study provides the scientific basis for the apparent coal-type dependence observed for Hg0 oxidation occurring across the SCR reactors in the field.  相似文献   

3.
Abstract

Efforts to develop multipollutant control strategies have demonstrated that adding certain oxidants to different classes of Ca-based sorbents leads to a significant improvement in elemental Hg vapor (Hg0), SO2, and NOx removal from simulated flue gases. In the study presented here, two classes of Ca-based sorbents (hydrated limes and silicate compounds) were investigated. A number of oxidizing additives at different concentrations were used in the Ca-based sorbent production process. The Hg0, SO2, and NOx capture capacities of these oxidant-enriched sorbents were evaluated and compared to those of a commercially available activated carbon in bench-scale, fixed-bed, and fluid-bed systems. Calcium-based sorbents prepared with two oxidants, designated C and M, exhibited Hg0 sorp-tion capacities (~100 μg/g) comparable to that of the activated carbon; they showed far superior SO2 and NOx sorption capacities. Preliminary cost estimates for the process utilizing these novel sorbents indicate potential for substantial lowering of control costs, as compared with other processes currently used or considered for control of Hg0, SO2, and NOx emissions from coal-fired boilers. The implications of these findings toward development of multipollutant control technologies and planned pilot and field evaluations of more promising multipollutant sorbents are summarily discussed.  相似文献   

4.
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   

5.
ABSTRACT

This article presents the results of an industrial-scale study (on 400 MWe lignite fired unit) of simultaneous NOx, SO2, and HgT removal in FGD absorber with oxidant injection (NaClO2) into flue gas. It was confirmed that the injection of sodium chlorite upstream the FGD (Flue Gas Desulfurization) absorber oxidize NO to NO2, Hg0 to Hg2+, and enhancing NOx and HgT removal efficiency from exhaust gas in FGD absorber. Mercury removal efficiency grows with the rise of degree of oxidation NO to NO2 and was limited by the phenomenon of re-emission. For NOx removal the most critical parameters is slurry pH and temperature. There was no negative effect on sulfur dioxide removal efficiency caused by oxidant injection in tested FGD absorber. Based on the data provided, NOx and HgT emissions can be reduced by adjusting the FGD absorber operating parameters combined with oxidant injection.  相似文献   

6.
湿式烟气脱硫系统同时脱汞研究   总被引:3,自引:0,他引:3  
研究表明,湿法烟气脱硫装置(WFGD)可去除烟气中绝大部分Hg2+,但对单质汞的吸收效果不明显,因此研究提高湿法烟气脱硫系统中单质汞的氧化率的方法对控制汞的排放具有重要意义。综述了WFGD及在此系统中各种添加剂的脱汞性能,认为在添加剂中,气态的臭氧、液态的次氯酸和氯化钠稀溶液、 黄磷乳浊液、氢硫化钠溶液及EDTA的汞去除效果较好,且不会被SO2大量消耗,可在WFGD系统实现同时脱硫脱汞;而气态的氯气,液态的K2S2O8溶液虽然也有较好的汞去除效果,但因易被SO2或亚硫酸盐溶液消耗,当在WFGD系统中用其氧化单质汞时,需要对脱硫塔进行分层或其他改造,使烟气中的SO2被吸收后再控制汞,提高经济性。  相似文献   

7.
Sodium hypochlorite (NaClO) has been widely used as a chemical additive for enhancing nitrogen oxide (NOx; NO + NO2), sulfur dioxide (SO2), and mercury (Hg0) removals in a wet scrubber. However, they are each uniquely dependent on NaClO(aq) pH, hence making the simultaneous control difficult. In order to overcome this weakness, we sprayed low liquid-to-gas (L/G) ratio (0.1 L/Nm3) of NaClO(aq) to vaporize quickly at 165 °C. Results have shown that the maximized NOx, SO2, and Hg0 removals can be achieved at the pH range between 4.0 and 6.0. When NOx and Hg0 coexist with SO2, in addition, their removals are significantly enhanced by reactions with solid and gaseous by-products such as NaClO(s), NaClO2(s), OClO, ClO, and Cl species, originated from the reaction between SO2 and NaClO(aq). We have also demonstrated the feasibility of this approach in the real flue gases of a combustion plant and observed 50%, 80%, and 60% of NOx, SO2, and Hg0 removals, respectively. These findings led us to conclude that the spray of NaClO(aq) at a relatively high temperature at which the sprayed solution can vaporize quickly makes the simultaneous control of NOx, SO2, and Hg0 possible.

Implications: The simple spray of NaClO(aq) at temperatures above 165 °C can cause the simultaneous removal of gaseous NOx, SO2, and Hg0 by its quick vaporization. Their maximized removals are achieved at the pH range between 4.0 and 6.0. NOx and Hg0 removals are also enhanced by gaseous and solid intermediate products generated from the reaction of SO2 with NaClO(aq). The feasibility of this approach has been demonstrated in the real flue gases of a combustion plant.  相似文献   


8.

Activated carbon was one of the main adsorptions utilized in elemental mercury (Hg0) removal from coal combustion flue gas. However, the high cost and low physical adsorption efficiency of activated carbon injection (ACI) limited its application. In this study, an ultra-high efficiency (nearly 100%) catalyst sorbent-Sex/Activated carbon (Sex/AC) was synthesized and applied to remove Hg0 in the simulated flue gas, which exhibited 120 times outstanding adsorption performance versus the conventional activated carbon. The Sex/AC reached 17.98 mg/g Hg0 adsorption capacity at 160 °C under the pure nitrogen atmosphere. Moreover, it maintained an excellent mercury adsorption tolerance, reaching the efficiency of Hg0 removal above 85% at the NO and SO2 conditions in a bench-scale fixed-bed reactor. Characterized by the multiple methods, including BET, XRD, XPS, kinetic and thermodynamic analysis, and the DFT calculation, we demonstrated that the ultrahigh mercury removal performance originated from the activated Se species in Sex/AC. Chemical adsorption plays a dominant role in Hg0 removal: Selenium anchored on the surface of AC would capture Hg0 in the flue gas to form an extremely stable substance-HgSe, avoiding subsequent Hg0 released. Additionally, the oxygen-containing functional groups in AC and the higher BET areas promote the conversion of Hg0 to HgO. This work provided a novel and highly efficient carbon-based sorbent -Sex/AC to capture the mercury in coal combustion flue gas.

Selenium-modified porous activated carbon and the interface functional group promotes the synergistic effect of physical adsorption and chemical adsorption to promote the adsorption capacity of Hg0.

  相似文献   

9.
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   

10.
ABSTRACT

The capture of elemental mercury (Hg0) and mercuric chloride (HgCl2) by three types of calcium (Ca)-based sor-bents was examined in this bench-scale study under conditions prevalent in coal-fired utilities. Ca-based sorbent performances were compared with that of an activated carbon. Hg0 capture of about 40% (nearly half that of the activated carbon) was achieved by two of the Ca-based sorbents. The presence of sulfur dioxide (SO2) in the simulated coal combustion flue gas enhanced the Hg0 capture from about 10 to 40%. Increasing the temperature in the range of 65-100 °C also caused an increase in the Hg0 capture by the two Ca-based sorbents. Mercuric chloride (HgCl2) capture exhibited a totally different pattern. The presence of SO2 inhibited the HgCl2 capture by Ca-based sorbents from about 25 to less than 10%. Increasing the temperature in the studied range also caused a decrease in HgCl2 capture. Upon further pilot-scale confirmations, the results obtained in this bench-scale study can be used to design and manufacture more cost-effective mercury sorbents to replace conventional sorbents already in use in mercury control.  相似文献   

11.
ABSTRACT

At conditions typical of a bag filter exposed to a coal-fired flue gas that has been adiabatically cooled with water, calcium hydroxide and calcium silicate solids were exposed to a dilute, humidified gas stream of nitrogen dioxide (NO2) and sulfur dioxide (SO2) in a packed-bed reactor. A prior study found that NO2 reacted readily with surface water of alkaline and non-alkaline solids to produce nitrate, nitrite, and nitric oxide (NO). With SO2 present in the gas stream, NO2 also reacted with S(IV), a product of SO2 removal, on the exterior of an alkaline solid. The oxidation of S(IV) to S(VI) by oxygen reduced the availability of S(IV) and lowered removal of NO2. Subsequent acidification of the sorbent by the removal of NO2 and SO2 facilitated the production of NO. However, the conversion of nitrous acid to sulfur-nitrogen compounds reduced NO production and enhanced SO2 removal. A reactor model based on empirical and semi-empirical rate expressions predicted rates of SO2 removal, NO2 removal, and NO production by calcium silicate solids. Rate expressions from the reactor model were inserted into a second program, which predicted the removal of SO2 and NOx by a continuous process, such as the collection of alkaline solids in a baghouse. The continuous process model, depending upon inlet conditions, predicted 30-40% removal for NO and 50-90% removal for SO2. These x 2 results are relevant to dry scrubbing technology for combined SO2 and NOx removal that first oxidizes NO to NO2 by the addition of methanol into the flue duct.  相似文献   

12.
用于气态零价汞转化的催化剂研究   总被引:4,自引:0,他引:4  
零价汞的高效去除是燃煤烟气汞污染控制过程中的关键环节。为了促进烟气中的零价汞转化为易于去除的氧化态汞,分别考察了在有HCl存在时,几种过渡金属氧化物(Cu、Fe、Mn、Co和Zr)对零价汞氧化的催化作用,以筛选出性能较好的催化组分;为提高催化剂的抗SO2性能,分别尝试了利用几种金属元素(Sr、Ce、W和Mo)对催化剂进行掺杂改性的方法。结果表明,锰氧化物的催化作用最好,其最佳使用温度在573 K左右;SO2对零价汞的催化氧化有明显抑制作用,在无SO2及1 400 mg/m3SO2时锰催化剂对零价汞催化氧化效率分别为93%和78%。而Mo改性的锰氧化物催化剂的抗硫性能大幅提高,在1 400 mg/m3SO2存在的情况下其对零价汞的催化氧化效率可达到90%以上,较其他改性元素高。  相似文献   

13.
Abstract

Bench-scale testing of elemental mercury (Hg0) sorption on selected activated carbon sorbents was conducted to develop a better understanding of the interaction among the sorbent, flue gas constituents, and Hg0. The results of the fixed-bed testing under simulated lignite combustion flue gas composition for activated carbons showed some initial breakthrough followed by increased mercury (Hg) capture for up to ~4.8 hr. After breakthrough, the Hg in the effluent stream was primarily in an oxidized form (>90%). Aliquots of selected activated carbons were exposed to simulated flue gas containing Hg0 vapor for varying time intervals to explore surface chemistry changes as the initial breakthrough, Hg capture, and oxidation occurred. The samples were analyzed by X-ray photoelectron spectroscopy to determine changes in the abundance and forms of sulfur, chlorine, oxygen, and nitrogen moieties as a result of interactions of flue gas components on the activated carbon surface during the sorption process. The data are best explained by a competition between the bound hydrogen chloride (HCl) and increasing sulfur [S(VI)] for a basic carbon binding site. Because loss of HCl is also coincident with Hg breakthrough or loss of the divalent Hg ion (Hg2+), the competition of Hg2+ with S(VI) on the basic carbon site is also implied. Thus, the role of the acid gases in Hg capture and release can be explained.  相似文献   

14.
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   

15.
This study examines gaseous chlorinated species generated from the reaction of sulfur dioxide (SO2) with sodium chlorite powder (NaClO2(s)) to obtain insight into the propensity of this process to enhance NO and Hg0 oxidation. A packed bed reactor containing NaClO2(s) was used and the reaction temperature was set to 130 °C. Initially, we determined that the presence of SO2 enhances the oxidation of NO and Hg0 by reaction with NaClO2(s). We then introduced NO2 into the gas mixture as a radical scavenger and determined that the chlorinated species generated by the reaction of SO2 with NaClO2(s) are OClO, Cl, ClO, and Cl2. Based on these results, we suggest that such gaseous chlorinated ones are responsible for the enhancement of NO and Hg0 oxidation.  相似文献   

16.
Fenton氧化法同时脱硫脱硝的实验研究   总被引:1,自引:0,他引:1  
应用Fenton液相氧化吸收法进行同时脱硫脱硝实验。首先,利用单因素实验,分别考察了H2O2浓度、Fe2+投加量、初始pH值、UV照射和温度对脱硫脱硝的影响。结果表明,SO2和NO去除率随着H2O2浓度和Fe2+投加量的增大而提高;初始pH对SO2和NO的去除有较大影响;UV能促进SO2和NO的净化;温度对脱硫效率影响不大,但对NO的去除有显著作用,适当升温可以提高脱硝效率。随后,考察了SO2对NO去除率的影响。通过单独脱硝和同时脱硫脱硝的对比实验发现,SO2的加入对NO的去除有一定的促进作用,Fenton法可同时获得起始约80%的脱硝效率和98%以上的脱硫效率。  相似文献   

17.
ABSTRACT

Analysis of Hg speciation in combustion flue gases is often accomplished in standardized sampling trains in which the sample is passed sequentially through a series of aqueous solutions to capture and separate oxidized Hg (Hg2+) and elemental Hg (Hg0). Such methods include the Ontario Hydro (OH) and the Alkaline Mercury Speciation (AMS) methods, which were investigated in the laboratory to determine whether the presence of Cl2 and other common flue gas species can bias the partitioning of Hg0 to front impingers intended to isolate Hg2+ species. Using only a single impinger to represent the front three impingers for each method, it was found that as little as 1-ppm Cl2 in a simulated flue gas mixture led to a bias of approximately 10-20% of Hg0 misreported as Hg2+ for both the OH and the AMS methods. Experiments using 100-ppm Cl2 led to a similar bias in the OH method, but to a 30-60% bias in the AMS method. These false readings are shown to be due to liquid-phase chemistry in the impinger solutions, and not necessarily to the gas-phase reactions between Cl2 and Hg as previously proposed. The pertinent solution chemistry causing the interference  相似文献   

18.
Potential source contribution function (PSCF) was employed to study the source receptor relationships for 14 chemical species (Mn, SO42−, Zn, Al, Fe, Cu, Cr, Ni, Cd, NO3, NH4+, K+, Mg2+,and Pb) found in precipitation collected at Lewes, Delaware. This study identified areas of the Eastern United States as possible emission source areas that could have contributed to the 14 element concentrations observed at Lewes. The identified regions in the Eastern United States generally coincide well with known emission source areas. The likely emission sources for these chemical species include oil- and coal-fired power plants, incinerators, motor vehicles, and iron and steel mills.  相似文献   

19.
20.
The measurement of hydrochloric acid (HCl) on a continuous basis in coal-fired plants is expected to become more important if HCl standards become implemented as part of the Federal Mercury and Air Toxics Standards (MATS) standards that are under consideration. For this study, the operational performance of three methods/instruments, including tunable diode laser absorption spectroscopy (TDLAS), cavity ring down spectroscopy (CRDS), and Fourier transform infrared (FTIR) spectroscopy, were evaluated over a range of real-world operating environments. Evaluations were done over an HCl concentration range of 0–25 ppmv and temperatures of 25, 100, and 185 °C. The average differences with respect to temperature were 3.0% for the TDL for values over 2.0 ppmv and 6.9% of all concentrations, 3.3% for the CRDS, and 4.5% for the FTIR. Interference tests for H2O, SO2, and CO, CO2, and NO for a range of concentrations typical of flue gases from coal-fired power plants did not show any strong interferences. The possible exception was an interference from H2O with the FTIR. The instrument average precision over the entire range was 4.4% for the TDL with better precision seen for concentrations levels of 2.0 ppmv and above, 2.5% for the CRDS, and 3.5% for the FTIR. The minimum detection limits were all on the order of 0.25 ppmv, or less, utilizing the TDL values with a 5-m path. Zero drift was found to be 1.48% for the TDL, 0.88% for the CRDS, and 1.28% for the FTIR.

Implications: This study provides an evaluation of the operational performance of three methods/instruments, including TDL absorption spectroscopy (TDLAS), cavity ring down spectroscopy (CRDS), and FTIR spectroscopy, for the measurement of hydrochloric acid (HCl) over a range of real-world operating environments. The results showed good instrument accuracy as a function of temperature and no strong interferences for flue gases typical to coal-fired power plants. The results show that these instruments would be viable for the measurement of HCl in coal-fired plants if HCl standards become implemented as part of the Federal Mercury and Air Toxics Standards (MATS) standards that are under consideration.  相似文献   


设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号