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1.
This paper reported mercury speciation and emissions from five coal-fired power stations in China. The standard Ontario Hydro Method (OHM) was used into the flue gas mercury sampling before and after fabric filter (FF)/electrostatic precipitator (ESP) locations in these coal-fired power stations, and then various mercury speciation such as Hg0, Hg2+ and HgP in flue gas, was analyzed by using EPA method. The solid samples such as coal, bottom ash and ESP ash, were analyzed by DMA 80 based on EPA Method 7473. Through analysis the mercury speciation varied greatly when flue gas went through FF/ESP. Of the total mercury in flue gas, the concentration of Hg2+ is in the range of 0.11–14.76 μg/N m3 before FF/ESP and 0.02–21.20 μg/N m3 after FF/ESP; the concentration of Hg0 ranges in 1.18–33.63 μg/N m3 before FF/ESP and 0.77–13.57 μg/N m3 after FF/ESP, and that of HgP is in the scope of 0–12.11 μg/N m3 before FF/ESP and 0–0.54 μg/N m3 after FF/ESP. The proportion of Hg2+ ranges from 4.87%–50.93% before FF/ESP and 2.02%–75.55% after FF/ESP, while that of Hg0 is between 13.81% – 94.79% before FF/ESP and 15.69%–98% after FF/ESP, with that of HgP is in the range of 0%–45.13% before FF/ESP and 0%–11.03% after FF/ESP. The mercury in flue gas mainly existed in the forms of Hg0 and Hg2+. The concentrations of chlorine and sulfur in coal and flue gas influence the species of Hg that are formed in the flue gas entering air pollution control devices. The concentrations of chlorine, sulfur and mercury in coal and the compositions of fly ash had significant effects on mercury emissions.  相似文献   

2.
Mercury in coal and its emissions from coal-fired boilers is a topic of primary environmental concern in the United States and Europe. The predominant forms of mercury in coal-fired flue gas are elemental (Hg0) and oxidized (Hg2+, primarily as HgCl2). Because Hg2+ is more condensable and far more water soluble than Hg0, the wide variability in mercury speciation in coal-fired flue gases undermines the total mercury removal efficiency of most mercury emission control technologies. It is important therefore to have an understanding of the behaviour of mercury during coal combustion and the mechanisms of mercury oxidation along the flue gas path. In this study, a temperature programmed decomposition technique was applied in order to acquire an understanding of the mode of decomposition of mercury species during coal combustion. A series of mercury model compounds were used for qualitative calibration. The temperature appearance range of the main mercury species can be arranged in increasing order as HgCl2 < HgS < HgO < HgSO4. Different fly ashes with certified and reference values for mercury concentration were used to evaluate the method. This study has shown that the thermal decomposition test is a newly developed efficient method for identifying and quantifying mercury species from coal combustion products.  相似文献   

3.
Mercury (Hg) is a toxic trace element which is emitted mostly in gas phase during coal combustion, although some Hg compounds may be retained in the fly ashes depending on the characteristics of the ashes and process conditions. To improve the retention of Hg in the fly ashes a good knowledge of the capture mechanism and Hg species present in the fly ashes is essential. The temperature programmed decomposition technique was chosen to identify the Hg species present in fly ashes obtained from two Pulverized Coal Combustion (PCC) plants and a Fluidized Bed Combustion (FBC) plant. The fly ashes were then used as Hg sorbents in a simulated flue gas of coal combustion and gasification. The Hg compounds found in the fly ash from the FBC plant after elemental mercury retention were mainly HgCl2 and HgSO4. The Hg species present in the two fly ashes from the two PCC plants were HgCl2 and Hg0. The Hg species formed in the coal gasification atmosphere was HgS for all three fly ashes. The only Hg compound identified in the fly ashes after the retention of mercury chloride was HgCl2.  相似文献   

4.
Speciation of As, Cr, Se and Hg under coal fired power station conditions   总被引:3,自引:0,他引:3  
Coal combustion from power stations is an important anthropogenic contributor of toxic trace elements to the environment. Some trace elements may be emitted in range of valencies, often with varying toxicity and bioavailability. Hence, determination of trace element speciation in coals and their combustion products is important for conducting comprehensive risk assessments of the emissions from coal-fired power stations. This study focuses on speciation of selected trace elements, As, Cr, and Se, in coal combustion products and Hg in flue gas, which were sampled at one Australian power station. Different analytical methods such as secondary ion mass spectrometry (SIMS), ion chromatography-inductively coupled plasma mass spectrometry (IC-ICPMS) and X-ray absorption near edge structure spectrometry (XANES) were used to determine trace element speciation in coal and ash samples. Results showed that As, Cr and Se are all present in a range of valency states in coal. Concentrations of As and Se in the bottom ash as well as the more toxic hexavalent chromium were less than the detection limits. The more toxic As3+ form in fly ash was at 10% of the total arsenic, while selenium was mainly found in Se4+ form. Hexavalent chromium (Cr6+) in fly ash was 2.7% of the total fly ash chromium. Mercury speciation in flue gas was determined using the Ontario Hydro sampling train and analysis technique. Approximately 58% of the total mercury in flue gas was released in the elemental form (Hg0), which, among all mercury species, has the highest residence time in the environment due to lower solubility. This work summarises the performance of the selected analytical techniques for speciation of trace elements.  相似文献   

5.
Mercury speciation and emission from two Chinese coal‐fired power stations equipped with flue gas desulfurization device were investigated. Research results reveal that Hg0 is the main form in the flue gas in Plant 1; Hg2+ is the main form in the flue gas in Plant 2. Most of mercury was emitted to the atmosphere, which was about 77–98%, and the elemental mercury released to atmosphere ranged 73–94% approximately. A pot of mercury is adsorbed by bottom ash, electrostatic precipitator (ESP) ash, and gypsum in Plant 1. However, most mercury, the scale of which is 75–83.2%, is collected by ESP ash, and only 7.0–12.2% mercury is emitted to the atmosphere in Plant 2. The mercury removal by NID semi‐desulfurization system is higher than wet flue gas desulfurization (WFGD) desulfurization system.  相似文献   

6.
A multi-field electrostatic precipitator (ESP) and a two-stage condensing heat exchanger (CHX®) have been added to the pilot scale Vertical Combustion Research Facility (VCRF) in CETC-O to further research into integrated emissions control for coal fired power plants. A series of combustion trials were conducted on the VCRF with three different coals (bituminous, sub-bituminous and lignite) to study mercury distribution and speciation at various VCRF locations. Results showed that, with the bituminous coal, as the flue gas cools down from 700 to 200 °C, 80% of total mercury in the gas phase existed in oxidized form and 20% in elemental form. For sub-bituminous and lignite coals, elemental mercury was the dominant form throughout the system. Analysis of deposited ash samples showed that oxidized mercury can be absorbed on carbon-rich ash deposits, although overall only a very small percentage of total mercury was absorbed on the ash. The potential of the CHX® at removing mercury from the flue gas was also explored. Results indicated that, using wet scrubbing, the CHX® was able to remove 98% of oxidized mercury. Though elemental mercury went through the system unabated, it is suggested that, with appropriate agent to oxidize elemental mercury in the CHX®, it is conceivable to use CHX® to remove both oxidized and elemental mercury. Finally, mercury balance was performed and good mercury balance was obtained across the VCRF, validating our sampling procedures and analysis methods.  相似文献   

7.
Heterogeneous oxidation of mercury in simulated post combustion conditions   总被引:2,自引:0,他引:2  
Heterogeneous mercury oxidation was studied by exposing whole fly ash samples and magnetic, nonmagnetic, and size-classified fly ash fractions to elemental mercury vapor in simulated flue gas streams. Fly ash from sub-bituminous Wyodak-Anderson PRB coal and bituminous Blacksville coal were used. Scanning electron microscopy, X-ray diffraction, thermogravimetric analyses, and BET N2 isothermal sorption analyses were performed to characterize the fly ash samples. Mercury speciation downstream from the ash was determined using the Ontario Hydro method. Results showed that the presence of fly ash was critical for mercury oxidation, and the surface area of the ash appears to be an important parameter. However, for a given fly ash, there were generally no major differences in catalytic oxidation potential between different fly ash fractions. This includes fractions enriched in unburned carbon and iron oxides. The presence of NO2, HCl, and SO2 resulted in greater levels of mercury oxidation, while NO inhibited mercury oxidation. The gas matrix affected mercury oxidation more than the fly ash composition.  相似文献   

8.
Among various pollutants, mercury has a significant impact on the environment, human beings, and wildlife with its different forms, namely, elemental mercury (Hg0), oxidized mercury (Hg2+), and particle-bound mercury (Hgp). Mercury dispersions mainly occur from coal burning, which is the world's major energy source. Among the three forms, Hg2+ and Hgp are relatively easy to remove from the flue gas by employing typical air pollution control devices; on the other hand, Hg0 is difficult to remove. Various methods are available to detain elemental mercury. Recent developments in mercury removal options, especially during the last years, are reviewed. Main concentration has been focused on the removal methods of elemental mercury by novel sorbents and catalytic systems. A current challenge is to develop novel nanomaterials meeting rigorous requirements (easy separation, recyclability, and cost-effectiveness) for eventual exploitation.  相似文献   

9.
Mercury emissions from coal-fired power plants account for 40% of the anthropogenic mercury emissions in the U.S. The speciation of mercury largely determines the amount of mercury capture in control equipments. Conversion of insoluble Hg0 into more soluble Hg2+ facilitates its removal in scrubbers. Past studies suggest that an added supply of OH radicals possibly enhance the mercury oxidation process. This study demonstrates that the application of H2O2, as source of OH radicals, accelerates the oxidation of Hg0 into Hg2+. A detailed kinetic reaction mechanism was compiled and the reaction pathways were established to analyze the effect of H2O2 addition. The optimum temperature range for the oxidation was 480–490 °C. The sensitivity analysis of the reaction mechanism indicates that the supply OH radicals increase the formation of atomic Cl, which accelerates the formation of HgCl2 enhancing the oxidation process. Also, the pathway through HOCl radical, generated by the interactions between chlorine and H2O2 was prominent in the oxidation of Hg0. The flue gas NO was found to be inhibiting the Hg0 oxidation, since it competed for the supplied H2O2. Studying the interactions with the other flue gas components and the surface chemistry with particles in the flue gas could be important and may improve the insight into the post combustion transformation of mercury in a comprehensive way.  相似文献   

10.
Bench-scale investigations indicate that NO, NO2, hematite (α-Fe2O3), maghemite (γ-Fe2O3), and HCl promote the conversion of gaseous elemental mercury (Hg0) to gaseous oxidized mercury (Hg2+) and/or particle-associated mercury (Hg[p]) in simulated coal combustion flue gases. In this investigation, the effects of NOx, α-Fe2O3, γ-Fe2O3, and HCl on Hg transformations were evaluated by injecting them into actual coal combustion flue gases produced from burning subbituminous Absaloka and lignitic Falkirk coals in a 7-kW down-fired cylindrical furnace. A bituminous Blacksville coal known to produce an Hg2+-rich combustion flue gas was also burned in the system. The American Society for Testing and Materials Method D6784-02 (Ontario Hydro method) or an online Hg analyzer equipped to measure Hg0 and total gaseous mercury (Hg[tot]) was used to monitor Hg speciation at the baghouse inlet (160–195 °C) and outlet (110–140 °C) locations of the system. As expected, the baseline Blacksville flue gas was composed predominantly of Hg2+ (Hg2+/Hg[tot]=0.77), whereas Absaloka and Falkirk flue gases contained primarily Hg0 (Hg0/Hg[tot]=0.84 and 0.78, respectively). Injections of NO2 (80–190 ppmv) at 440–880 °C and α-Fe2O3 (15 and 6 wt.%) at 450 °C into Absaloka and Falkirk coal combustion flue gases did not significantly affect Hg speciation. The lack of Hg0 to Hg2+ conversion suggests that components of Absaloka and Falkirk combustion flue gases and/or fly ashes inhibit heterogeneous Hg0–NOx–α-Fe2O3 reactions or that the flue gas quench rate in the 7-kW system is much different in relation to bench-scale flue gas simulators.An abundance of Hg2+, HCl, and γ-Fe2O3 in Blacksville flue gas and the inertness of injected α-Fe2O3 with respect to heterogeneous Hg0 oxidation in Absaloka and Falkirk flue gases suggested that γ-Fe2O3 catalyzes Hg2+ formation and that HCl is an important Hg0 reactant. The filtration of Absaloka and Falkirk combustion flue gases at 150 °C through fabric filters with ≈60 g/m2 γ-Fe2O3 indicated that about 30% of the Hg0 in Absaloka and Falkirk flue gases was converted to Hg2+ and/or Hg(p). HCl injection (100 ppmv) into the Absaloka combustion flue gas converted most of the Hg0 to Hg2+, whereas HCl injection into the Falkirk flue gas converted most of the Hg0 and Hg2+ to Hg(p). Additions of γ-Fe2O3 and HCl did not have a synergistic effect on Hg0 oxidation. The filtration of Absaloka and Falkirk flue gases through much greater fabric filter loadings of 475 g/m2 γ-Fe2O3 essentially doubled the baghouse Hg[tot] removal efficiency to about 50%. Results from this investigation demonstrate the importance of evaluating potential Hg0 reactants and oxidation catalysts in actual coal combustion flue gases.  相似文献   

11.
Converting elemental mercury into divalent compound is one of the most important steps for mercury abatement from coal fired flue gas. The oxidation of elemental mercury was investigated in this paper using dielectric barrier discharge (DBD) non-thermal plasma (NTP) technology at room temperature. Effects of different flue gas components like oxygen, moisture, HCl, NO and SO2 were investigated. Results indicate that active radicals including O, O3 and OH all contribute to the oxidation of elemental mercury. Under the conditions of 5% O2 in the simulated flue gas, about 90.2% of Hg0 was observed to be oxidized at 3.68 kV discharge voltage. The increase of discharge voltage, O2 level and H2O content can all improve the oxidation rate, individually. With O2 and H2O both existed, there is an optimal moisture level for the mercury oxidation during the NTP treatment. In this test, the observed optimal moisture level was around 0.74% by volume. Hydrogen chloride can promote the oxidation of mercury due to chlorine atoms produced in the plasma process. Both NO and SO2 have inhibitory effects on mercury oxidation, which can be attributed to their competitive consumption of O3 and O.  相似文献   

12.
The present study investigated the variation of mercury (Hg) speciation within the air pollution control devices (APCDs) in bituminous coal-fired power plants. The effect of selective catalytic reduction (SCR) system, which is mainly installed for NOx removal, on elemental Hg (Hg0) oxidation and enhancement of Hg removal within APCDs, was studied. Hg speciations in flue gas at the inlet and outlet of each APCDs, such as SCR, cold-side electrostatic precipitator (CS-ESP) and flue gas desulphurization (FGD), were analyzed. Sampling and analysis were carried out according to Ontario Hydro Method (OHM). Overall Hg removal efficiency of APCDs, on average, was about 61% and 47% with and without SCR system, respectively. In the flue gas, Hg was mainly distributed in gaseous (elemental and oxidized) form. The oxidized to elemental Hg partitioning coefficient increased due to oxidation of Hg0 across the SCR system and decreased due to the removal of oxidized Hg (Hg2+) across a wet FGD system. Hg0 oxidation across the SCR system varied from 74% to 7% in tested coal-fired power plants. The comparative study shows that the installation of an SCR system increased Hg removal efficiency and suppressed the reemission of captured Hg0 within a wet FGD system.  相似文献   

13.
Ye Zhuang 《Fuel》2007,86(15):2351-2359
Pilot-scale experiments were conducted to investigate mercury transformations in coal flue gas when firing subbituminous coal with a CaCl2 additive. Cofiring the CaCl2 additive with the subbituminous coal resulted in approximately 50% oxidized mercury, as a result of reactive chlorine species formed in coal flue gas, compared to the dominance of elemental mercury in the baseline flue gas. The mercury data indicate that mercury-flue gas chemistry reactions may occur at fairly high temperatures (>400 °C) in chlorine-enriched flue gas. Field tests were conducted to further demonstrate the impact of cofiring CaCl2 on the eventual fate of mercury. These tests were completed on a 650-MW subbituminous coal-fired power plant equipped with selective catalytic reduction (SCR), a fabric filter (FF), and a wet scrubber. Overall mercury removals across the SCR-FF-wet scrubber system ranged from 75% to 96% with 200-800 ppm (coal basis) chlorine addition compared to 18-32% during baseline operations. Field data indicate that the SCR enhanced mercury oxidation, possibly as a result of the supplemental formation of reactive chlorine species and the aid of the SCR catalyst. As a result, most of the mercury in the flue gas was in an oxidized state and was removed in the downstream wet scrubber, indicating that cofiring CaCl2 is an effective mercury control approach for a subbituminous coal-fired plant equipped with an SCR and wet scrubber.  相似文献   

14.
Mercury emissions from six coal-fired power plants in China   总被引:1,自引:0,他引:1  
Mercury emission field measurements based on the Ontario Hydro Method (OHM) were conducted for six coal-fired power plants in China. The mercury mass balances for the six power plants varied from 100.3% to 139.5% of the input coal mercury for the whole system. About 0.02%–1.2% of the mercury remained in the bottom ash. In the first five power plants equipped with pulverized coal boiler, most of the mercury was emitted from the stack to the atmosphere. The plants with Electrostatic Precipitator (ESP) system emitted more Hg0 than Hg2+, while the plants with the Fabric Filter (FF) emitted less Hg0 than Hg2+. Virtually all of the HgP enter the ESP or the FF was removed. The FF systems had better Hg0 and Hg2+ removal efficiencies than the ESP systems. The flue gas desulfurization (FGD) system removed up to 78.0% of Hg2+ and only 3.14% of Hg0 in the flue gas, while 8.94% of the original mercury in the coal was removed by the FGD system. The average mercury removal efficiencies of the ESP systems was 11.5%, that of the FF systems was 52.3% and that of the combined ESP + FGD system was 13.7%, much lower than the average removal efficiencies of pollution control device systems in US plants which have been used in previous studies of Chinese mercury emission inventory. Hg0, rather than Hg2+ as assumed in previous estimates, has been found to be the dominant species emitted in the atmosphere. The average emission factor was found to be 4.70 g/TJ (10.92 bl/Tbtu), which is much higher than for US plants burning bituminous coals due to the high mercury content in the Chinese coal and the low mercury removal efficiency of air pollution control devices of power plants.  相似文献   

15.
This paper presents the results of field measurements on mercury speciation in six power plants of China by applying the Ontario hydro method. During the tests, flue gas was sampled simultaneously before and after particulate control devices (electrostatic precipitator and fabric filter baghouse) along with the pulverized coal, bottom ash and fly ash sampling. The amount of oxidized mercury in gas phase before and after ESP/FF suggests that mercury oxidation after combustion is a kinetically controlled process. The comparison of mercury speciation in different power plant indicates a clear relationship with coal type, especially the chlorine concentration and the basic ash compositions in coal. Both of the factors are analyzed quantitatively in this study. A new parameter C (ratio of chlorine in coal to base/acid ratio) has been introduced to evaluate the co-effect of the two factors above on mercury speciation.  相似文献   

16.
A novel silica–titania (SiO2–TiO2) nanocomposite has been developed to effectively capture elemental mercury (Hg0) under UV irradiation. Previous studies under room conditions showed over 99% Hg0 removal efficiency using this nanocomposite. In this work, the performance of the nanocomposite on Hg0 removal was tested in simulated coal-fired power plant flue gas, where water vapor concentration is much higher and various acid gases, such as HCl, SO2, and NOx, are present. Experiments were carried out in a fix-bed reactor operated at 135 °C with a baseline gas mixture containing 4% O2, 12% CO2, and 8% H2O balanced with N2. Results of Hg speciation data at the reactor outlet demonstrated that Hg0 was photocatalytically oxidized and captured on the nanocomposite. The removal efficiency of Hg0 was found to be significantly affected by the flue gas components. Increased water vapor concentration inhibited Hg0 capture, due to the competitive adsorption of water vapor. Both HCl and SO2 promoted the oxidation of Hg0 to Hg(II), resulting in higher removal efficiencies. NO was found to have a dramatic inhibitory effect on Hg0 removal, very likely due to the scavenging of hydroxyl radicals by NO. The effect of NO2 was found to be insignificant. Hg removal in flue gases simulating low rank coal combustion products was found to be less than that from high rank coals, possibly due to the higher H2O concentration and lower HCl and SO2 concentrations of the low rank coals. It is essential, however, to minimize the adverse effect of NO to improve the overall performance of the SiO2–TiO2 nanocomposite.  相似文献   

17.
The important step for increasing gaseous elemental mercury (Hg0) removal in wet scrubber systems is altering the chemical form of the Hg0 to a water‐soluble oxidized species. This work focuses on the removal of elemental mercury from simulated flue gas by aqueous sodium chlorite in a bubble reactor. The effects of initial oxidizing solution concentration, reaction temperature, pH and mercury concentration in the inlet of the reactor on mercury oxidative absorption in sodium chlorite were investigated. The results indicate that higher concentrations of sodium chlorite favor Hg0 removal, with a greater efficiency observed in acidic than in alkaline solution. High temperature inhibits Hg0 absorption in aqueous sorbent when the reaction temperature is lower than ca. 40 °C, and the removal efficiency increases when the temperature is higher than that value. In conclusion, the major influencing factors on the levels of Hg0 removal are pH and chlorite concentration in solution.  相似文献   

18.
王帅  高继慧  吴燕燕  吴少华 《化工学报》2010,61(12):3251-3257
采用新型一体化脱硫工艺和循环流化床烟气脱硫工艺的脱硫灰为吸附剂,使用固定床反应器,在模拟烟气的条件下研究了两种半干法脱硫灰对汞的吸附及催化氧化特性。研究结果表明,吸附于脱硫灰表面的汞主要以Hg2+的形态存在,多数情况下,更高的汞氧化率伴随有更高的汞吸附率,HCl、Cl2、NO2在脱硫灰的催化作用下能有效氧化Hg0,且不同组分对Hg0的氧化作用可以累积,而NO和SO2抑制了脱硫灰对汞的吸附。脱硫灰中未燃尽碳和Fe2O3对脱硫灰吸附和催化氧化气态汞具有显著促进作用。汞吸附率和氧化率在使用两种脱硫灰作为吸附剂时均随温度升高先增大后减小,这是传质过程和反应速率共同作用的结果。  相似文献   

19.
The effect of porous structure and surface functionality on the mercury capacity of a fly ash carbon and its activated sample has been investigated. The samples were tested for mercury adsorption using a fixed‐bed with a simulated flue gas. The activated fly ash carbon sample has lower mercury capacity than its precursor fly ash carbon (0.23 vs. 1.85 mg/g), although its surface area is around 15 times larger, 863 vs. 53 m2/g. It was found that oxygen functionality and the presence of halogen species on the surface of fly ash carbons may promote mercury adsorption, while the surface area does not seem to have a significant effect on their mercury capacity.  相似文献   

20.
循环流化床中烟气飞灰汞迁移规律   总被引:2,自引:0,他引:2       下载免费PDF全文
黄勋  程乐鸣  蔡毅  侯文慧  周劲松 《化工学报》2014,65(4):1387-1395
在小型热态循环流化床试验台上进行褐煤、烟煤、无烟煤燃烧试验,研究3种典型煤的烟气气态汞和飞灰颗粒汞迁移规律。试验结果表明:褐煤、烟煤、无烟煤在燃烧过程中,炉膛温度、空截面风速、给煤量以及煤颗粒大小变化时,汞元素在烟气和飞灰之间的迁移规律相似;降低炉膛密相区温度和增大炉膛空截面风速可促进烟气气态总汞HgT(g)迁移到飞灰颗粒汞Hg(p)中,同时也促进烟气气态零价汞Hg0(g)向烟气气态二价汞Hg2+(g)和Hg(p)转化;增加给煤量,烟气气态总汞HgT(g)和烟气气态零价汞Hg0(g)减少,飞灰颗粒汞Hg(p)含量增加,并且影响Hg0(g)的转化;选择合适的煤颗粒粒度可以促进Hg0(g)的转化以及HgT(g)向Hg(p)迁移。随燃烧工况的变化,3种煤HgT(g)、Hg(p)和Hg0(g)含量变化趋势相似,但含量相差较大,Hg0(g)占HgT(g)的比例y值也不同,其中无烟煤的y值高于烟煤和褐煤的y值。  相似文献   

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