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 15 毫秒
1.
Experiments were conducted in a fixed-bed reactor that contained a commercial catalyst, V2O5–WO3/TiO2, to investigate mercury oxidation in the presence of NO and O2. Mercury oxidation was improved by NO, and the efficiency was increased by simultaneously adding NO and O2. With NO and O2 pretreatment at 350°C, the catalyst exhibited higher catalytic activity for Hg0 oxidation, whereas NO pretreatment did not exert a noticeable effect. Decreasing the reaction temperature boosted the performance of the catalyst treated with NO and O2. Although NO promoted Hg0 oxidation at the very beginning, excessive NO counteracted this effect. The results show that NO plays different roles in Hg0 oxidation; NO in the gaseous phase may directly react with the adsorbed Hg0, but excessive NO hinders Hg0 adsorption. The adsorbed NO was converted into active nitrogen species (e.g., NO2) with oxygen, which facilitated the adsorption and oxidation of Hg0. Hg0 was oxidized by NO mainly by the Eley–Rideal mechanism. The Hg0 temperature-programmed desorption experiment showed that weakly adsorbed mercury species were converted to strongly bound ones in the presence of NO and O2.  相似文献   

2.
La2O3/Bi2O3 photocatalysts were prepared by impregnation of Bi2O3 with an aqueous solution of lanthanum precursor followed by calcination at different temperatures. The composite materials were used for the first time for the photocatalytic removal of Hg0 from a simulated flue gas under UV light irradiation. The results showed that the sample containing 6 wt.% La2O3 and calcined at 500°C has the highest dispersion of the active sites, which was promoted by the strong interaction with the support (i.e., the formation of Bi-O-La species). Since they are fully accessible on the surface, the material also exhibits excellent optical properties while the heterojunction formed in La2O3/Bi2O3 promotes the separation and migration of photoelectron-hole pairs and thus Hg0 oxidation efficiency is enhanced. The effects of the various factors (e.g., the reaction temperature and composition of the simulated flue gas (i.e., O2, NO, H2O, and SO2)) on the efficiency of the Hg0 photocatalytic oxidation were investigated. The results demonstrated that O2 and SO2 enhanced the efficiency of the reaction while the reaction temperature, NO, and H2O had an inhibitory effect.  相似文献   

3.
A Ce_(0.3)TiO_xoxide carrier was synthesized via a sol–gel process,and Ce_(0.3)TiO_xsupported metal(M=Cd,Mn,Fe,W,Mo)oxide catalysts were prepared by the method of incipient-wetness impregnation.The catalysts were characterized by means of X-ray diffraction(XRD),Brunauer–Emmett–Teller(BET)analysis,scanning electron microscopy(SEM),transmission electron microscopy(TEM),Fourier transform infrared(FT–IR)spectroscopy,UV–Visdiffusereflectancespectroscopy(UV–VisDRS),and Temperature-programmed reduction with H_2(H_2-TPR).The catalytic activities for de-NO_(x )were evaluated by the NH_3-SCR reaction.Among all the catalysts tested,the 2 wt.%Cd/Ce_(0.3)TiO_xcatalyst exhibited the best NH_3-SCR performance,with a wide temperature window of 250–450°C for NO conversion above 90%.Moreover,the catalyst showed N_2 selectivity greater than 99%from 200 to 450°C.  相似文献   

4.
A novel ferruginous active absorbent, prepared by fly ash, industrial lime and the additive Fe(VI), was introduced for synchronous abatement of binary mixtures of SO2–NOx from simulated coal-fired flue gas. The synergistic action of various factors on the absorption of SO2 and NOx was investigated. The results show that a strong synergistic effect exists between Fe(VI) dose and reaction temperature for the desulfurization. It was observed that in the denitration process, the synergy of Fe(VI) dose and Ca/(S + N) had the most significant impact on the removal of NO, followed by the synergy of Fe(VI) and reaction temperature, and then the synergy of reaction temperature and flue gas humidity. A scanning electron microscope(SEM) and an accessory X-ray energy spectrometer(EDS)were used to observe the surface characteristics of the raw and spent absorbent as well as fly ash. A reaction mechanism was proposed based on chemical analysis of sulfur and nitrogen species concentrations in the spent absorbent. The Gibbs free energy, equilibrium constants and partial pressures of the SO2–NOx binary system were determined by thermodynamics.  相似文献   

5.
A novel ferruginous active absorbent, prepared by fly ash, industrial lime and the additive Fe(VI), was introduced for synchronous abatement of binary mixtures of SO2–NOx from simulated coal-fired flue gas. The synergistic action of various factors on the absorption of SO2 and NOx was investigated. The results show that a strong synergistic effect exists between Fe(VI) dose and reaction temperature for the desulfurization. It was observed that in the denitration process, the synergy of Fe(VI) dose and Ca/(S + N) had the most significant impact on the removal of NO, followed by the synergy of Fe(VI) and reaction temperature, and then the synergy of reaction temperature and flue gas humidity. A scanning electron microscope (SEM) and an accessory X-ray energy spectrometer (EDS) were used to observe the surface characteristics of the raw and spent absorbent as well as fly ash. A reaction mechanism was proposed based on chemical analysis of sulfur and nitrogen species concentrations in the spent absorbent. The Gibbs free energy, equilibrium constants and partial pressures of the SO2–NOx binary system were determined by thermodynamics.  相似文献   

6.
沈伯雄  陈建宏  蔡记  何川  李卓 《环境科学》2014,35(8):2890-2896
卤素改性材料对烟气中单质汞的去除具有较高的效率,黏土(膨润土)在我国分布广,资源丰富且廉价易得.为探究KI改性黏土对烟气中单质汞的脱除效率,以浸渍法制得了KI改性膨润土,研究了不同KI负载量、不同吸附温度及不同烟气氛围下,改性膨润土对Hg0的脱除效率和累积吸附量,并与原始膨润土进行对比.运用比表面分析(BET)、傅里叶红外光谱仪(FTIR)及热重分析法(TGA)等方法对材料的物理化学特性进行了分析.结果表明,KI改性大大提升膨润土对Hg0的脱除效率,并且Hg0的脱除效率随着KI负载量的加大而上升.温度提高了吸附剂吸附Hg0的性质,吸附剂主要表现为化学吸附.O2有利于吸附剂对Hg0的吸附.SO2对吸附剂吸附Hg0有轻微的促进作用,H2O的存在对吸附剂吸附Hg0具有很强的抑制作用.  相似文献   

7.
A series of cobalt doped TiO_2(Co-TiO_2) and Co Oxloaded TiO_2(Co/TiO_2) catalysts prepared by sol–gel and impregnation methods respectively were investigated on selective catalytic reduction with NH_3(NH_3-SCR) of NO. It was found that Co-TiO_2 catalyst showed more preferable catalytic activity at low temperature range. From characterization results of XRD,TEM, Raman and FT-IR, Co species were proved to be doped into TiO_2 lattice by replaced Ti atoms. After being characterized and analyzed by NH_3-TPD, PL, XPS, EPR and DRIFTS, it was found that the better NH_3-SCR activities of Co-TiO_2 catalysts, compared with Co/TiO_2 catalyst, were ascribed to the formation of more oxygen vacancies which further promoted the production of more superoxide ions(O-2). The superoxide ions were crucial for the formation of low temperature SCR reaction intermediates(NO-3) by reacting with adsorbed NO molecule. Therefore, these aspects were responsible for the higher low temperature NH_3-SCR activity of Co-TiO_2 catalysts.  相似文献   

8.
Experiments were conducted in a fixed-bed reactor containing a commercial V2O5/WO3/TiO2 catalyst to investigate mercury oxidation in the presence of HCl and O2. Mercury oxidation was improved significantly in the presence of HCl and O2, and the Hg0 oxidation efficiencies decreased slowly as the temperature increased from 200 to 400°C. Upon pretreatment with HCl and O2 at 350°C, the catalyst demonstrated higher catalytic activity for Hg0 oxidation. Notably, the effect of pretreatment with HCl alone was not obvious. For the catalyst treated with HCl and O2, better performance was observed with lower reaction temperatures. The results showed that both HCl and Hg0 were first adsorbed onto the catalyst and then reacted with O2 following its adsorption, which indicates that the oxidation of Hg0 over the commercial catalyst followed the Langmuir–Hinshelwood mechanism. Several characterization techniques, including Hg0 temperature-programmed desorption (Hg-TPD) and X-ray photoelectron spectroscopy (XPS), were employed in this work. Hg-TPD profiles showed that weakly adsorbed mercury species were converted to strongly bound species in the presence of HCl and O2. XPS patterns indicated that new chemisorbed oxygen species were formed by the adsorption of HCl, which consequently facilitated the oxidation of mercury.  相似文献   

9.
The elemental mercury removal abilities of three different zeolites (NaA, NaX, HZSM-5) impregnated with iron(III) chloride were studied on a lab-scale fixed-bed reactor. X-ray diffraction, nitrogen adsorption porosimetry, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and temperature programmed desorption (TPD) analyses were used to investigate the physicochemical properties. Results indicated that the pore structure and active chloride species on the surface of the samples are the key factors for physisorption and oxidation of Hg0, respectively. Relatively high surface area and micropore volume are beneficial to efficient mercury adsorption. The active Cl species generated on the surface of the samples were effective oxidants able to convert elemental mercury (Hg0) into oxidized mercury (Hg2 +). The crystallization of NaCl due to the ion exchange effect during the impregnation of NaA and NaX reduced the number of active Cl species on the surface, and restricted the physisorption of Hg0. Therefore, the Hg0 removal efficiencies of the samples were inhibited. The TPD analysis revealed that the species of mercury on the surface of FeCl3–HZSM-5 was mainly in the form of mercuric chloride (HgCl2), while on FeCl3–NaX and FeCl3–NaA it was mainly mercuric oxide (HgO).  相似文献   

10.
Elemental mercury (Hg^0) in flue gases can be efficiently captured by mercury chloride (HgCl2) solution. However, the absorption behaviors and the influencing effects are still poorly understood. The mechanism of Hg^0 absorption by HgCl2 and the factors that control the removal were studied in this paper. It was found that when the mole ratio of Cl^- to HgCl2 is 10:1, the Hg^0 removal efficiency is the highest. Among the main mercury chloride species, HgCl3^- is the most efficient ion for Hg^0 removal in the HgCl2 absorption system when moderate concentrations of chloride ions exist. The Hg^0 absorption reactions in the aqueous phase were investigated computationaIIy using Moller-Plesset perturbation theory. The calculated Gibbs free energies and energy barriers are in excellent agreement with the results obtained from experiments. In the presence of SO3^2- and SO2, Hg^2+ reduction occurred and Hg^0 removal efficiency decreased. The reduced Hg^0 removal can be controlled through increased chloride concentration to some degree. Low pH value in HgCla solution enhanced the Hg^0 removal efficiency, and the effect was more significant in dilute HgCl2 solutions. The presence of SO4^2- and NO3^- did not affect Hg^0 removal by HgCl2.  相似文献   

11.
Due to the ever-tightening regulation on mercury emission in recent decades, there is an urgent need to develop novel materials for the removal of elemental mercury at coal-fired power plants. In this study, a series of MoS2 quantum dots (QDs)-based MoS2/HKUST-1 composite materials were prepared. It is found that MoS2 QDs were encapsulated by HKUST-1 and enhanced the crystallinity and specific surface area of HKUST-1. The MoS2/HKUST-1 showed excellent performance in catalytic oxidation of Hg0 as compared with pristine HKUST-1. It is found that surface layer of lattice oxygens is active and participates in Hg0 oxidation, while the consumption of surface oxygens then leads to the formation of oxygen vacancies on the surface. These vacancies are effective in the adsorption and dissociation of O2, which subsequently participates in the oxidation of Hg0. Moreover, the study on the influence of commonly seen gas components, such as SO2, NO, NH3 and H2O, etc., on Hg0 oxidation demonstrated that synergistic effects exist among these gas species. It is found that the presence of NO promotes the oxidation of Hg0 using oxygen as the oxidant.  相似文献   

12.
Selective catalytic reduction (SCR) denitration may increase the emission of NH4+ and NH3. The removal and transformation characteristics of ammonium sulfate aerosols and ammonia slip during the wet flue gas desulfurization (WFGD) process, as well as the effect of desulfurization parameters, were investigated in an experimental system equipped with a simulated SCR flue gas generation system and a limestone-based WFGD system. The results indicate that the ammonium sulfate aerosols and ammonia slip in the flue gas from SCR can be partly removed by slurry scrubbing, while the entrainment and evaporation of desulfurization slurry with accumulated NH4+ will generate new ammonium-containing particles and gaseous ammonia. The ammonium-containing particles formed by desulfurization are not only derived from the entrainment of slurry droplets, but also from the re-condensation of gaseous ammonia generated by slurry evaporation. Therefore, even if the concentration of NH4+ in the desulfurization slurry is quite low, a high level of NH4+ was still contained in the fine particles at the outlet of the scrubber. When the accumulated NH4+ in the desulfurization slurry was high enough, the WFGD system promoted the conversion of NH3 to NH4+ and increased the additional emission of primary NH4+ aerosols. With the decline of the liquid/gas ratio and flue gas temperature, the removal efficiency of ammonia sulfate aerosols increased, and the NH4+ emitted from entrainment and evaporation of the desulfurization slurry decreased. In addition, the volatile ammonia concentration after the WFGD system was reduced with the decrease of the NH4+ concentration and pH values of the slurry.  相似文献   

13.
Me/SAPO-34 (Me = Mn, Ni, Co) series of catalysts were prepared by a wetness impregnation method and investigated for the selective catalytic reduction of nitrogen oxides with ammonia (NH3-SCR). Among them, Mn/SAPO-34 catalyst was found as the most promising candidate based on its superior low-temperature activity. The catalysts were characterized by X-ray diffraction (XRD), transmission electron microscopy images (TEM), nuclear magnetic resonance (NMR), X-ray photoelectron spectroscopy (XPS), temperature programmed reduction and desorption (TPR and TPD), and diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) of NH3/NOx adsorption. Mn/SAPO-34 is obviously different from Ni/SAPO-34 and Co/SAPO-34 in the active species state and distribution. Surface MnOx species which play an essential role in NO oxidation and NO2 adsorption, act as better active sites than nickel and cobalt mostly in the form of the aluminates and silicates.  相似文献   

14.
MnxCe1- xO2(x: 0.3–0.9) prepared by Pechini method was used as a catalyst for the thermal catalytic oxidation of formaldehyde(HCHO). At x = 0.3 and 0.5, most of the manganese was incorporated in the fluorite structure of Ce O2 to form a solid solution. The catalytic activity was best at x = 0.5, at which the temperature of 100% removal rate is the lowest(270°C). The temperature for 100% removal of HCHO oxidation is reduced by approximately 40°C by loading 5 wt.% Cu Oxinto Mn0.5Ce0.5O2. With ozone catalytic oxidation, HCHO(61 ppm) in gas stream was completely oxidized by adding 506 ppm O3 over Mn0.5Ce0.5O2 catalyst with a GHSV(gas hourly space velocity) of 10,000 hr-1at 25°C. The effect of the molar ratio of O3 to HCHO was also investigated. As O3/HCHO ratio was increased from 3 to 8, the removal efficiency of HCHO was increased from 83.3% to 100%. With O3/HCHO ratio of 8, the mineralization efficiency of HCHO to CO2 was 86.1%. At 25°C, the p-type oxide semiconductor(Mn0.5Ce0.5O2) exhibited an excellent ozone decomposition efficiency of 99.2%,which significantly exceeded that of n-type oxide semiconductors such as Ti O2, which had a low ozone decomposition efficiency(9.81%). At a GHSV of 10,000 hr-1, [O3]/[HCHO] = 3 and temperature of 25°C, a high HCHO removal efficiency(≥ 81.2%) was maintained throughout the durability test of 80 hr, indicating the long-term stability of the catalyst for HCHO removal.  相似文献   

15.
A series of MnM/palygorskite (PG) (M = La, W, Mo, Sb, Mg) catalysts was prepared by the wetness co-impregnation method for low-temperature selective catalytic reduction (SCR) of NO with NH3. Conversion efficiency followed the order Sb > Mo > La > W > Mg. A combination of various physico-chemical techniques was used to investigate the influence of Sb-modified Mn/PG catalysts. MnSb0.156/PG catalyst showed highest NO conversion at low temperatures in the presence of SO2 which reveals that addition of Sb oxides effectively enhances the SCR activity of catalysts. A SO2 step-wise study showed that MnSb0.156/PG catalyst displays higher durable resistance to SO2 than Mn/PG catalyst, where the sulfating of active phase is greatly inhibited after Sb doping. Scanning electron microscopy and X-ray diffraction results showed that Sb loading enhances the dispersion of Mn oxides on the carrier surface. According to the results of characterization analyses, it is suggested that the main reason for the deactivation of Mn/PG is the formation of manganese sulfates which cause the permanent deactivation of Mn-based catalysts. For Sb-doped Mn/PG catalyst, SOx ad-species formed were mainly combined with SbOx rather than MnOx. This preferential interaction between SbOx and SO2 effectively shields the MnOx as active species from being sulfated by SO2 resulting in the improvement of SO2 tolerance on Sb-added catalyst. Multiple information support that, owing to the addition of Sb, original formed MnOx crystallite has been completely transformed into highly dispersed amorphous phase accounting for higher SCR activity.  相似文献   

16.
燃煤电厂采用SCR(选择性催化还原)脱硝过程消耗大量的氨,同时存在氨逃逸和氨排放问题.为了掌握超低排放燃煤机组的氨排放程度、脱硝氨逃逸情况以及各环保设施对氨的协同脱除能力,为燃煤电厂氨减排政策制定和氨减排技术研发提供支持.在京津冀大气污染传输通道城市中选取11个城市中的14台机组,采用例如DL/T 260—2012《燃煤电厂烟含脱硝装置性能验收试验规范》的标准方法用稀硫酸吸收烟气中的氨再结合分光光度测试方法,对环保设施多个位置的烟气中氨进行浓度测试.结果表明:①氨排放浓度介于0.05~3.27 mg/m3之间,平均约0.95 mg/m3,通过烟气排入大气中氨的浓度不高;②测试的14台机组中有7台机组(约50%)脱硝氨逃逸值高于设计值(2.28 mg/m3),说明脱硝氨逃逸超过设计值呈普遍现象,个别电厂脱硝氨逃逸严重,氨逃逸亟待解决;③环保设施对逃逸氨具有较好的协同脱除能力,平均脱除率约为64.86%.建议对于SCR脱硝氨逃逸严重的机组,对SCR出口烟道截面氮氧化物(NOx)实施网格式测试,在此基础上实施精细化精准喷氨、优化流场、提高SCR脱硝运行水平(或采用专业化运维),从源头上减少氨耗量,降低系统能耗和氨排放.   相似文献   

17.
废茶活性炭脱硫脱硝性能的应用研究   总被引:1,自引:0,他引:1  
宋磊  张彬  邓文 《环境科学》2014,35(10):3674-3682
为探讨废茶活性炭对于SO2和NO脱除作用的制约因素,分别考察了材料孔径结构、石墨化程度及表面结构对其脱硫脱硝性能的影响,同时研究了其吸附机制及动力学过程.结果表明,较高的石墨化程度是影响材料脱硫性能的主要因素,微孔径较小且含氮碱性基团较高时有利于SO2的脱除;发达的中孔结构是制约NO脱除效率的关键因素,含氮碱性基团对NO的脱除具有一定的促进作用;烟气中SO2和NO共存时,材料的脱硫脱硝性能均有所降低,氧气和水蒸气的加入能够改善其脱硫脱硝效率;废茶活性炭在无水环境下对于SO2和NO的吸附作用均以物理吸附为主,水蒸气的存在促进了材料对SO2的化学吸附;通过动力学模型的拟合发现,Bangham吸附模型能够很好地描述材料脱硫脱硝的动力学过程,其R2均高于0.989,材料对于SO2和NO的吸附速率常数均随氧气和水蒸气的加入而减小.  相似文献   

18.
The adsorption characteristics of virgin and potassium permanganate modified lignite semi-coke (SC) for gaseous Hg0 were investigated in an attempt to produce more effective and lower price adsorbents for the control of elemental mercury emission. Brunauer-Emmett-Teller (BET) measurements, X-ray powder diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) were used to analyze the surface physical and chemical properties of SC, Mn-SC and Mn-H-SC before and after mercury adsorption. The results indicated that potassium permanganate modification had significant influence on the properties of semi-coke, such as the specific surface area, pore structure and surface chemical functional groups. The mercury adsorption efficiency of modified semi-coke was lower than that of SC at low temperature, but much higher at high temperature. Amorphous Mn7+, Mn6+ and Mn4+ on the surface of Mn-SC and Mn-H-SC were the active sites for oxidation and adsorption of gaseous Hg0, which oxidized the elemental mercury into Hg2+ and captured it. Thermal treatment reduced the average oxidation degree of Mnx+ on the surface of Mn-SC from 3.80 to 3.46. However, due to the formation of amorphous MnOx, the surface oxidation active sites for gaseous Hg0 increased, which gave Mn-H-SC higher mercury adsorption efficiency than that of Mn-SC at high temperature.  相似文献   

19.
Fly ash is a potential alternative to activated carbon for mercury adsorption. The effects of physicochemical properties on the mercury adsorption performance of three fly ash samples were investigated. X-ray fluorescence spectroscopy, X-ray photoelectron spectroscopy, and other methods were used to characterize the samples. Results indicate that mercury adsorption on fly ash is primarily physisorption and chemisorption. High specific surface areas and small pore diameters are beneficial to efficient mercury removal. Incompletely burned carbon is also an important factor for the improvement of mercury removal efficiency, in particular. The C-M bond, which is formed by the reaction of C and Ti, Si and other elements, may improve mercury oxidation. The samples modified with CuBr2 , CuCl 2 and FeCl3 showed excellent performance for Hg removal, because the chlorine in metal chlorides acts as an oxidant that promotes the conversion of elemental mercury (Hg0) into its oxidized form (Hg2+). Cu2+ and Fe3+ can also promote Hg 0 oxidation as catalysts. HCl and O2 promote the adsorption of Hg by modified fly ash, whereas SO2 inhibits the Hg adsorption because of competitive adsorption for active sites. Fly ash samples modified with CuBr2 , CuCl2 and FeCl3 are therefore promising materials for controlling mercury emissions.  相似文献   

20.
不同光源下TiO2/ACF同时脱硫脱硝实验研究   总被引:1,自引:0,他引:1  
韩静  赵毅 《环境科学》2009,30(4):997-1002
实验室制备了负载型二氧化钛光催化剂TiO2/ACF,利用自行设计的光催化反应器,在紫外和可见2种光源下进行了同时脱硫脱硝试验,确定了最佳的试验条件,比较了2种不同光源下的脱除效率.结果表明,烟气中氧含量、反应温度、烟气含湿量、光照强度等是影响光催化的主要因素,在紫外光源的照射下,负载型TiO2/ACF光催化剂脱除SO2和NO的效率分别达到99.7%和64.3%,在可见光源的照射下,负载型TiO2/ACF光催化剂脱除SO2和NO的效率分别达到97.5%和49.6%, 5次平行试验结果表明,平行数据的标准偏差S较小.通过反应后吸收液的离子色谱分析,推测了2种不同光源下同时脱硫脱硝的反应机制.  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