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1.
The effect of halogen acids HCl, HBr and HI on mercury conversion was studied in a laboratory-scale SCR reactor using simulated flue gases, and is presented here. Two types of commercially available SCR catalysts, Honeycomb and Plate type catalysts, were used in these studies. HBr and HI both had shown much stronger effects on mercury conversion than HCl. Both HBr and HI oxidized more than 85% of the gas phase mercury at a low concentration of 2 ppm. The age of the catalyst and the type of catalyst also have an effect on mercury conversion. A larger extent of mercury oxidation was observed in the presence of a Honeycomb catalyst than with the Plate catalyst.  相似文献   

2.
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   

3.
Parametric experiments were carried out to study the interactions of mercury, SO3, and injected activated carbon (AC) in a coal flue gas stream. The levels of SO3 vapor in flue gas were altered by individually varying flue gas temperature, moisture, or sodium fume injection in the flue gas. Meanwhile, mercury emissions with AC injection (ACI) upstream of an electrostatic precipitator (ESP) were evaluated under varied SO3 concentrations. SO3 measurements using a condensation method indicated that low temperature, high moisture content, and sodium fume injection in flue gas shifted SO3 partitioning from the vapor to particulate phase, subsequently improving mercury capture with ACI. 0.08 g/m3 of DARCO® Hg-LH injection only provided approximately 20% mercury reduction across the ESP in a bituminous coal flue gas containing 28 ppm SO3, but mercury capture was increased to 80% when the SO3 vapor concentration was lowered less than 2 ppm. Experimental data clearly demonstrate that elevated SO3 vapor is the key factor that impedes mercury adsorption on AC, mainly because SO3 directly competes against mercury for the same binding sites and overwhelmingly consumes all binding sites.  相似文献   

4.
Z.H. Wang  A. Ehn  Z.S. Li  J. Bood  K.F. Cen 《Fuel》2010,89(9):2346-130
Direct ozone (O3) injection is a promising flue-gas treatment technology based on oxidation of NO and Hg into soluble species like NO2, NO3, N2O5, oxidized mercury, etc. These product gases are then effectively removed from the flue gases with the wet flue gas desulfurization system for SO2. The kinetics and mixing behaviors of the oxidation process are important phenomena in development of practical applications. In this work, planar laser-induced fluorescence (PLIF) of NO and NO2 was utilized to investigate the reaction structures between a turbulent O3 jet (dry air with 2000 ppm O3) and a laminar co-flow of simulated flue gas (containing 200 ppm NO), prepared in co-axial tubes. The shape of the reaction zone and the NO conversion rate along with the downstream length were determined from the NO-PLIF measurements. About 62% of NO was oxidized at 15d (d, jet orifice diameter) by a 30 m/s O3 jet with an influence width of about 6d in radius. The NO2 PLIF results support the conclusions deduced from the NO-PLIF measurements.  相似文献   

5.
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   

6.
The performance of V2O5/TiO2-based commercial SCR catalyst for the oxidation of gaseous elemental mercury (Hg0) with respect to reaction conditions was examined to understand the mechanism of Hg0 oxidation on SCR catalyst. It was observed that a much larger amount of Hg0 adsorbed on the catalyst surface under oxidation condition than under SCR condition. The activity of commercial SCR catalyst for Hg0 oxidation was negligible in the absence of HCl, regardless of reaction conditions. The presence of HCl in the reactant gases greatly increased the activity of SCR catalyst for the oxidation of Hg0 to oxidized mercury (Hg2+) such as HgCl2 under oxidation condition. However, the effect of HCl on the oxidation of Hg0 was much less under SCR condition than oxidation condition. The activity for Hg0 oxidation increased with the decrease of NH3/NO ratio under SCR condition. This might be attributed to the strong adsorption of NH3 prohibiting the adsorption of HCl which was vital species promoting the oxidation of Hg0 on the catalyst surface under SCR condition.  相似文献   

7.
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   

8.
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   

9.
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   

10.
Ye Zhuang  Chuanmin Chen  John Pavlish 《Fuel》2009,88(9):1692-1697
Mercury control technologies are often associated with adding halogens to the flue gas to enhance oxidation of elemental mercury. The present research was to evaluate the corrosion characteristics of iron in a flue gas containing bromine to simulate mercury control applications in coal-fired utility plants. An AISI 1008 cold rolled steel was exposed to a synthetic flue gas (7.1 vol% O2, 14.3 vol% CO2, 2.0 vol% H2O, 51 ppmv HBr, 510 ppmv SO2, 51 ppmv NOx, and the balance N2). Exposure times ranged from 30 days to 6 months. Metal coupons were exposed with simulated flue gases at 300°, 150°, and 80 F (149°, 66°, and 27 °C), respectively. The corroded coupons were analyzed using scanning electron microscope and micrometer measurements to determine the deposit chemistry and corrosion loss. The corrosion products consisted mainly of iron oxides and iron bromide. A mechanism for HBr corrosion is suggested. Bromine dew point corrosion took place on metal surfaces at temperatures below or close to the dew point of HBr, while active oxidation occurred at higher temperatures.  相似文献   

11.
Feng-Yim Chang  Ming-Yen Wey 《Fuel》2009,88(9):1563-1571
This study investigated the activity of Rh/Al2O3 and Rh-Na/Al2O3 catalysts for polycyclic aromatic hydrocarbons (PAHs) removal and the influence of particulates, heavy metals, and acid gases (SO2 and HCl) on the performance of catalysts. The experiments were carried out in a laboratory-scale waste incineration system. Experimental results show that the destruction removal efficiency (DRE) of PAHs by Rh/Al2O3 and Rh-Na/Al2O3 catalysts were 80% and 59%, respectively when the flue gas did not contain any pollutants. The concentrations of PAHs increased by using a Rh/Al2O3 catalyst when the flue gas contained Cd, Pb, and SO2 and also increased by using a Rh-Na/Al2O3 catalyst when the flue gas contained particulates, Cd, and HCl. Adding Na to the Rh/Al2O3 catalyst can inhibit the increases of 3-4 ring PAHs when the flue gas contained Pb. The influence of acid gases on the performance of the Rh/Al2O3 and Rh-Na/Al2O3 catalysts followed the sequence SO2 > HCl > SO2 + HCl. The activity of the catalysts for PAHs removal was significantly suppressed by increased concentrations in particulates and Cd, yet promoted by a high Pb concentration. The results of ESCA analysis indicated that the presence of Cd and Pb did not change the chemical states of Rh and Na, but the presence of SO2 and HCl did.  相似文献   

12.
The heterogeneous mercury reaction mechanism, reactions among elemental mercury (Hg0) and simulated flue gas across laboratory-scale selective catalytic reduction (SCR) reactor system was studied. The surface of SCR catalysts used in this study was analyzed to verify the proposed reaction pathways using transmission electron microscopy with energy dispersive X-ray analyses (TEM-EDX) and X-ray photoelectron spectroscopy (XPS). The Langmuir–Hinshelwood mechanism was proven to be most suitable explaining first-layer reaction of Hg0 and HCl on the SCR catalyst. Once the first layer is formed, successive layers of oxidized mercury (HgCl2) are formed, making a multi-layer structure.  相似文献   

13.
CuCl2-SCR catalysts prepared by an improved impregnation method were studied to evaluate the catalytic performance for gaseous elemental mercury (Hg0) oxidation in simulated flue gas. Hg0 oxidation activity of commercial SCR catalyst was significantly improved by the introduction of CuCl2. Nitrogen adsorption, XRD, XRF and XPS were used to characterize the catalysts. The results indicated that CuCl2 was well loaded and highly dispersed on the catalyst surface, and that CuCl2 played an important role for Hg0 catalytic oxidation. The effects of individual flue gas components on Hg0 oxidation were also investigated over CuCl2-SCR catalyst at 350 oC. The co-presence of NO and NH3 remarkably inhibited Hg0 oxidation, while this inhibiting effect was gradually scavenged with the decrease of GHSV. Further study revealed the possibility of simultaneous removal of Hg0 and NO over CuCl2-SCR catalyst in simulated flue gas. The mechanism of Hg0 oxidation was also investigated.  相似文献   

14.
《Fuel》2005,84(14-15):1968-1974
Removal of Hg0 vapor from the simulated coal combustion flue gases with a commercial activated carbon was investigated using H2S. This method is based on the reaction of H2S and Hg over the adsorbents. The Hg0 removal experiments were carried out in a conventional flow type packed bed reactor system in the temperature range of 80–150 °C using simulated flue gases having the composition of Hg0 (4.9 ppb), H2S (0–20 ppm), SO2 (0–487 ppm), CO2 (10%), H2O (0–15%), O2 (0–5%), N2 (balance gas). The following results were obtained: in the presence of both H2S and SO2, Hg removal was favored at lower temperatures (80–100 °C). At 150 °C, presence of O2 was indispensable for Hg0 removal from H2S–SO2 flue gas system. It is suggested that the partial oxidation of H2S with O2 to elemental sulfur (H2S+1/2O2=Sad+H2O) and the Clause reaction (SO2+2H2S=3Sad+2H2O) may contribute to the Hg0 removal over activated carbon by the following reaction: Sad+Hg=HgS. The formation of elemental sulfur on the activated carbon was confirmed by a visual observation.  相似文献   

15.
The present review paper highlights on the recent progress in Japan on the hot gas cleanup of HCl, H2S and NH3 in raw fuel gas for coal-based, combined cycle power generation technologies. It has been shown that NaAlO2, prepared by mixing Na2CO3 solution with Al2O3 sol, can reduce HCl in an air-blown gasification gas from the initial 200 ppm to < 1 ppm at 400 °C, and it is tolerable for 200 ppm H2S. With regard to the removal of H2S, studies on the stability and durability of ZnFe2O4 sorbent in a simulated fuel gas have indicated the presence of an optimal operation temperature from the viewpoint of the suppression of both vaporization of metallic Zn and carbon formation from CO. High-performance TiO2-supported ZnFe2O4, which can decrease 1000 ppm H2S to < 1 ppm at 450 °C and 1 MPa, has been developed by the homogeneous precipitation method using a mixture of SiO2 sol and an aqueous solution of Zn and Fe nitrates, followed by mixing with TiO2. Although this sorbent is regenerable and durable, the sorption ability should be improved in a syngas-rich fuel gas from an O2-blown gasifier. A novel method to prepare carbon-supported ZnFe2O4 and CaFe2O4 by impregnating the corresponding nitrate solution with brown coal has been proposed, and the large desulfurization capacity of almost 100% has been achieved in the removal of 4000 ppm H2S around 450 °C. The present authors have demonstrated that an Australian limonite rich in α-FeOOH is practically feasible as the catalyst material for the decomposition of 2000 ppm NH3 in a syngas-rich gas of 25 vol.% H2/50 vol.% CO at 750 °C, because small amounts of H2O and CO2 added to the gas can work efficiently for inhibiting carbon deposition from the CO.  相似文献   

16.
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   

17.
Feng-Yim Chang  Ming-Yen Wey 《Fuel》2010,89(8):1919-1927
SO2 and HCl are major pollutants emitted from waste incineration processes. Both pollutants are difficult to remove completely and can enter the catalytic reactor. In this work, the effects of SO2 and HCl on the performance of Rh/Al2O3 and Rh-Na/Al2O3 catalysts for NO removal were investigated in simulated waste incineration conditions. The characterizations of the catalysts were analyzed by BET, SEM/EDS, XRD, and ESCA. Experimental results indicated the 1%Rh/Al2O3 catalyst was significantly deactivated for NO and CO conversions when SO2 and HCl coexisted in the flue gas. The addition of between 2 and 10 wt.% Na promoted the activity of the 1%Rh/Al2O3 catalyst for NO removal, but decreased the CO oxidation and BET surface area. The catalytic activity for NO removal was inhibited by HCl as a result of the formation of RhCl3. Adding Na to the Rh/Al2O3 catalyst decreased the inhibition of SO2 because of the formation of Na2SO4, which was observed in the XRD and ESCA analyses. SEM mapping/EDS showed that more S was residual on the surface of the Rh-Na/Al2O3 catalyst than Cl.  相似文献   

18.
Recent developments in novel sorbents for flue gas clean up   总被引:4,自引:0,他引:4  
Coal combustion is one of the most important energy sources for electricity generation, but also produces airborne pollutants. The amount of SO2 and NOx for example, is in the order of hundreds to thousands of ppm, and tens to hundreds of ppm, respectively, while Hg in flue gases could be up to tens to hundreds of ppb. Flue gas desulphurization technology is already in place for SO2 removal, and new sorbents such as zeolites are being investigated for such an application. NOx can be removed by selective catalytic reduction with various catalysts. Mercury is the hardest to remove due to its persistent nature and relatively low concentration in flue gases. New sorbents have also been developed for mercury removal applications. A current trend in flue gas emission control is to remove Hg, NOx and SO2 simultaneously. Various catalytic sorbents have been investigated to remove two or more of these pollutants concurrently. This article reviews recent developments made for emission control of coal-fired power plant flue gases using novel sorbents to target individual or multiple pollutants.  相似文献   

19.
A promising technology has been developed to capture and remove elemental mercury species from coal-fired power plants. Powerspan Corp. has licensed the technology and initiated a bench and pilot test program to develop the Photochemical Oxidation, or PCO™, process for commercial application with subbituminous and lignite fuels.The process has the potential to serve as a low cost mercury oxidation technology that will facilitate elemental mercury removal in a downstream SO2 scrubber, wet electrostatic precipitator (WESP), or baghouse. It uses 254-nm (nanometer) ultraviolet light from a mercury lamp to produce an excited state mercury species in the flue gas, leading to oxidation of elemental mercury. This paper presents results of Powerspan's initial bench-scale testing on a simulated flue gas stream. Preliminary testing conducted in Powerspan's bench-scale facility showed greater than 90% oxidation and removal of elemental mercury. The process also has potential to serve as a low cost method for the removal of mercury from waste incinerator flue gases.  相似文献   

20.
No-Kuk Park  Gi Bo Han  Tae Jin Lee  Ki Jun Yoon 《Fuel》2007,86(14):2232-2240
Claus reaction (2H2S + SO2 ↔ 3/nSn + 2H2O) was used to clean the gasified coal gas and the reactivity of several metal oxide-based catalysts on Claus reaction was investigated at various operating conditions. In order to convert H2S contained in the gasified coal gas to elemental sulfur during Claus reaction, the catalysts having the high activity under the highly reducing condition with the moisture should be developed. CeO2, ZrO2, and Ce1−xZrxO2 catalysts were prepared for Claus reaction and their reactivity changes due to the existence of the reducing gases and H2O in the fuel gas was investigated in this study. The Ce-based catalysts shows that their activity was deteriorated by the reduction of the catalyst due to the reducing gases at higher than 220 °C. Meanwhile, the effect of the reducing gases on the catalytic activity was not considerable at low temperature. The activities of all three catalysts were degraded on the condition that the moisture existed in the test gas. Specifically, the Ce-based catalysts were remarkably deactivated by their sulfation. The Ce-Zr-based catalyst had a high catalytic activity when the reducing gases and the moisture co-existed in the simulated fuel gas. The deactivation of the Ce-Zr-based catalyst was not observed in this study. The lattice oxygen of the Ce-based catalyst was used for the oxidation of H2S and the lattice oxygen vacancy on the catalyst was contributed to the reduction of SO2. ZrO2 added to the Ce-Zr-based catalyst improved the redox properties of the catalyst in Claus reaction by increasing the mobility of the lattice oxygen of CeO2.  相似文献   

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