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1.
采用臭氧氧化结合湿法喷淋对模拟玻璃窑炉烟气开展了同时脱硫脱硝实验研究.采用不同溶液(NaOH、Na2S)进行了喷淋实验.结果表明,保证溶液pH值在10以上,NaOH浓度对NOx脱除效率无影响,SO2的存在促进了NOx吸收.当O3/NO物质的量比为1.6、溶液NaOH浓度为0.5%时,NOx脱除效率可达70%,SO2脱除效率在99%以上.往喷淋液中添加Na2S,NOx脱除效率随Na2S浓度增加而提高,SO2的存在对NOx脱除效率无影响.当O3/NO物质的量比为1.2、溶液中NaOH浓度为0.5%、添加剂Na2S浓度为0.6%时,NOx脱除效率可达70%,SO2脱除效率在95%以上.60 min长时间运行实验证明,模拟烟气中的NOx经碱液和添加剂吸收后主要以NO-2的形式存在于喷淋液中,且NOx脱除效率不随溶液pH值的变化而变化.  相似文献   

2.
The Co-modified CeO2-TiO2 catalyst prepared by facile co-precipitation was used for efficient elemental mercury oxidation in flue gas. Results indicated that Co doping greatly enhanced the activity and SO2 resistance of the CeO2-TiO2 catalyst. In the presence of 5% O2, 500 ppm NO, 800 ppm SO2 and 3% H2O at 200 °C, the Hg0 removal efficiency of CeCo3/Ti could maintain at about 87% for a relatively long time. Characterizations of catalysts (BET, XRD, Raman spectroscopy, TEM, H2-TPR, O2-TPD, XPS, TG-MS and SO2-DRIFTS) were carried out to reveal the mechanism of Co modification on the redox ability, SO2 resistance and resultant mercury oxidation removal performance of catalyst. It was found that an interaction of Ce with Co promoted the dispersion of CeO2, increased chemisorbed oxygen concentration, and improved the oxygen storage capacity and the reducibility of catalyst, which was beneficial to the improvement of Hg0 oxidation removal. Hg0 would adsorb onto the catalyst and react with surface active oxygen species replenished by gas-phase O2 to be oxidized via Mars-Maessen mechanism. SO2 consumed the surface active oxygen species and resulted in the reduction of Ce4+ to Ce3+, which induced the deactivation of catalyst. The introduced Co in CeO2-TiO2 catalyst exerted the function of protecting Ce4+ from being poisoned by SO2 and thus promoted the sulfur resistance and Hg0 removal performance of the catalyst in the presence of SO2.  相似文献   

3.
Mn–TiO2 catalysts were utilized as an ozonation catalyst for the first time to study the simultaneous catalytic ozonation of Hg0 and NO at low flue gas temperatures. BET, SEM–EDS, XRD, XPS, H2-TPR, NO x -TPD and Hg0-TPD were used to characterize the catalysts. The Mn–TiO2 catalyst, in which the molar content of metal Mn was 60%, exhibited the best catalytic activities of Hg0 and NO oxidation, compared with other Mn–TiO2 catalysts. It was found that within the range of experiment, the catalytic ozonation efficiency of Hg0 and NO was higher than that of ozonation or catalytic oxidation. The results also showed that the presence of NO gas inhibited the catalytic ozonation of elemental mercury, and the inhibition was enhanced with the NO inlet concentration, while few elemental mercury molecules did promote the catalytic ozonation of NO. The addition of H2O vapor promoted the catalytic ozonation of Hg0 and NO. In addition, 0.6Mn–TiO2 catalyst demonstrated a good TOS and cyclic stability. The catalytic ozonation of NO and Hg0 on Mn–TiO2 catalyst likely followed the Langmuir–Hinshelwood mechanism, where the hydroxyl radicals reacted with adjacently adsorbed NO molecules and elemental mercury on catalyst surface.  相似文献   

4.
According to the basic research performed using a small size reactor at TRCRE of JAERI, the electron beam irradiation process was proved to be very effective for NOx, SO2 and HC removals from flue-gas of municipal waste incinerators. Based on this result, a pilot-plant was constructed for the demonstration of NOx, SO2 and HC removal performance using electron accelerator of maximum energy 0.95 MeV and maximum power 15kW.The pilot-plant was constructed at Matsudo City waste Disposal Center. The flue-gas of 1,000 Nm3/hr is guided from the waste incinerator flue-gas line of 30,000Nm3/hr to the pilot-plant to be processed by spraying Ca(OH)2 slurry or powder and irradiation with high-energy electron beam of the accelerator. NOx, SO2 and HC are removed simultaneously from the flue-gas by the enhanced reaction with Ca (OH)2 under irradiation.A brief explanation of the pilot-plant and preliminary results of the experiments are introduced in this paper.  相似文献   

5.
A series of modified porous activated carbon (AC) catalysts prepared by impregnation were investigated for the low-temperature (≤250°C) selective catalytic reduction (SCR) of NO x with NH3 with simultaneous removal of SO2. The effects of various preparation conditions and reaction conditions on NO and SO2 conversions were observed, such as support type, active components, copper loading, calcination temperature and presence of H2O and O2. The modified AC catalysts were characterized by BET, XRD, TG and TPX methods. The activity test results showed that the optimal catalyst is 15% Cu/WCSAC which can provide 52% NO conversion and 68% SO2 conversion simultaneously at 175°C with a space velocity of 30000 h?1, and the optimal calcination temperature was 500°C. The presence of H2O could inhibit NO conversion and promote the SO2 conversion. The effect of O2 (0–5%) was evaluated, and the NO and SO2 conversions were best when the concentration of O2 was 3%. Research demonstrated that Cu/WCSAC catalyst was a kind of potential catalysts due to the amorphous phase, high specific areas and high active ability.  相似文献   

6.
The Co–Mn/Ti–Ce catalyst prepared by sol–gel and impregnation method was evaluated for catalytic oxidation of Hg0 in the simulated flue gas compared with Co/TiO2 and Co–Mn/TiO2. The results showed that Co–Mn/Ti–Ce catalyst exhibited higher catalytic activity (around 93% Hg0 removal efficiency in the temperature of 150 °C with 6% O2, 400 ppm NO, 200 ppm SO2 and 3% H2O) than Co/TiO2 and Co–Mn/TiO2. Based on the characterization results of N2 adsorption–desorption, XRD, UV–Vis, XPS, H2-TPR and Hg-TPD, it could be concluded that the lower band gap, better reducibility and mercury adsorption capability and the presence of Co3+/Co2+, Mn4+/Mn3+ and Ce4+/Ce3+ redox couples as well as surface oxygen species contributed to the excellent Hg0 oxidation removal performance. In addition, well dispersion of active components and a synergetic effect among Co, Mn and Ce species might improve the activity further. A Mars–Maessen mechanism is thought to be involved in the Hg0 oxidation. The lattice oxygen derived from MnO x or CoO x would react with adsorbed Hg0 to form HgO and the consumption of lattice oxygen could be replenished by O2. For Co–Mn/Ti–Ce, MnO x?1 could be alternatively reoxidized by the lattice oxygen derived from adjacent CoO x and CeO x which is beneficial to the Hg0 oxidation.  相似文献   

7.
Polysulfonyl Amines. XXXVII. Preparation of Mercury Dimesylamides. Crystal and Molecular Structures of Hg[N(SO2CH3)2]2, Hg[{N(SO2CH3)2}2(DMSO)2], and Hg[{N(SO2CH3)2}2(HMPA)] Hg[N(SO2CH3)2]2 ( 1 ) and Hg2[N(SO2CH3)2]2 ( 2 a ) are formed as colourless, sparingly soluble precipitates when solutions of Hg(NO3)2 or Hg2(NO3)2 in dilute nitric acid are added to an aqueous HN(SO2CH3)2 solution. By a similar reaction, Hg2[N(SO2C6H4 ? Cl? 4)2]2 is obtained. 1 forms isolable complexes of composition Hg[N(SO2CH3)2]2 · 2 L with L = dimethyl sulfoxide (complex 3 a ), acetonitrile, dimethyl formamide, pyridine or 1,10-phenanthroline and a (1/1) complex Hg[N(SO2CH3)2]2 · HMPA ( 4 ) with hexamethyl phosphoramide. Attempted complexation of 2 a with some of these ligands induced formation of Hg0 and the corresponding HgII complexes. Crystallographic data (at -95°C) are for 1: space group 141/a, a = 990.7(2), c = 2897.7(8) pm, V = 2.844 nm3, Z = 8, Dx = 2.545Mgm?3; for 4a: space group P1 , a = 767.8(2), b = 859.2(2), c = 925.2(2)pm α = 68.44(2), β = 86.68(2), γ = 76.24(2)°, V = 0.551nm3, Z = 1, Dx = 2.113 Mgm?3; for 4: space group P21/c, a = 1041.3(3), b = 1545.4(3), c = 1542.5(3) pm, β = 100.30(2)°, V = 2.474nm3, Z = 4, Dx = 1.944Mgm3. The three compounds form molecular crystals. The molecular structures contain a linear or approximately linear, covalent NHgN moiety; the Hg? N distances and N? Hg? N angles are 206.7(4) pm and 176.3(2)° for 1, 207.2(2) pm and 180.0° for 3a, 205.7(4)/206.7(4) pm and 170.5(1)° for 4. In the complexes 3a and 4, the 0-ligands are bonded to the Hg atoms perpendicularly to the N? Hg? N axes, leading in 3a to a square-planar trans-(N2O2) coordination with Hg? 0 261.2(2) pm and N? Hg? O 92.3(1)/87.7(1)°, in 4 to a slightly distorted T-shaped (N2O) geometry with Hg? 0 246.2(4)pm and N? Hg? 0 96.7(1)/92.0(1)°. In all three structures, the primary coordination is extended to a severely distorted (N2O4) hexacoordination by the appropriate number of secondary, inter- and/or intramolecular Hg…?0 inter-actions (0 atoms from sulfonyl groups, Hg…?O distances in the range 280—300pm). The intramolecular Hg…?O interactions give rise to nearly planar four-membered [HgNSO] rings. The molecule of 1 has a two-fold axis through the bisector of the N? Hg? N angle, the molecule of 3a an inversion center at the Hg atom. The molecule of 4 has no symmetry.  相似文献   

8.
史光  朱繁  喻瑞 《分子催化》2023,37(4):405-418
氮氧化物(NOx)是一种重要的大气污染物, 它造成严重的环境问题, 同时威胁人类健康. 以钢铁烧结烟气为代表的固定源和以柴油机尾气为代表的移动源是氮氧化物的主要来源. 氨气选择性催化还原法(NH3-SCR)是目前最有效且应用最广泛的NOx脱除技术. 然而, 无论是固定源还是移动源上NH3-SCR催化剂, 都不可避免地会被SO2毒化, 造成催化剂失活, 限制了NH3-SCR技术的进一步应用. 因此, 研究NH3-SCR催化剂的SO2中毒机制以及提高催化剂的抗硫性能至关重要. 我们对固定源脱硝的金属氧化物和移动源上脱硝的Cu基分子筛这两类不同催化剂体系的SO2中毒机制的研究进展进行了介绍, 并对这两种催化剂上提高抗硫性能改性方法的研究进展进行了评述, 为未来的研究提供了参考.  相似文献   

9.
Mercury emission from coal combustion has been the fourth biggest pollutant in China, following the dusts, SO2 and NOX. The technology of non-thermal plasma has been widely studied for oxidizing gaseous elemental mercury at low temperature. In this paper, a new method of combining non-thermal plasma with calcium oxide was proposed to remove elemental mercury from simulated flue gas. The effects of non-thermal plasma, input energy, combination mode of plasma and calcium oxide on Hg0 removal were investigated in a wire-cylinder non-thermal plasma reactor, whose energy was supplied by a high voltage alternating current power. The peak voltage and energy of the non-thermal plasma were measured by an oscilloscope and a high voltage probe (1000:1). The results showed that most of Hg0 was converted to oxidized mercury in simulated flue gas by non-thermal plasma treatment. The Hg0 removal efficiency of CaO was improved remarkably strengthened by the non-thermal plasma, which was closely related to input energy, and the maximum mercury removal efficiency was about 80 % at an optimal input energy. Through temperature-programmed decomposition and desorption and energy dispersive spectroscopy analysis, the majority of mercury species on CaO surface were Hg2O and HgO3 rather than HgO. Therefore, it can be concluded that O3 plays an important role in Hg0 oxidation under the condition of non-thermal plasma.  相似文献   

10.
郭丽红  刘咏  孟明 《化学进展》2009,21(5):964-970
NOx 储存-还原(NSR)技术是最有前景的稀燃氮氧化物消除技术,自从日本丰田公司1996年首次提出NOx 储存还原这一概念后,一直受到研究者的广泛关注。本文综述了近十余年来NSR催化剂(PBA型、水滑石型、钙钛矿型)的研究进展,重点概述了目前比较公认的NOx储存-还原的反应路径,以及NSR催化剂的失活机制,包括H2O和CO2的负面影响,热失活和硫中毒问题,最后展望了NOx 储存还原技术未来的发展趋势。  相似文献   

11.
Composite supports CeO2-ZrO2-Al2O3 (CZA) and CeO2-ZrO2-Al2O3-La2O3 (CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperature-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Catalytic activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. They also have significant potential in industrial application because of their high performance and low cost.  相似文献   

12.
Hg2(CH3SO3)2: Synthesis, Crystal Structure, Thermal Behavior, and Vibrational Spectroscopy Colorless single crystals of Hg2(CH3SO3)2 are formed in the reaction of HgO, Hg, and HSO3CH3. In the monoclinic compound (I2/a, Z = 4, a=883.2(2), b=854.0(2), c=1188.9(2) pm, β = 92.55(2)°, Rall=0.0445) the Hg22+ ion is coordinated by two monodentate CH3SO3 anions. Further contacts Hg‐O occur in the range from 262 to 276 pm and lead to a linkage of the [Hg2(CH3SO3)2] units. The thermal analysis shows that Hg2(CH3SO3)2 decomposes at 300° yielding elemental mercury. The mass numbers of the species evolved lead to the assumtion that SO3, SO2, CO2, CO and H2CO are formed during the reaction. In the IR and the Raman spectrum the typical vibrations of the CH3SO3 ion are observed, the Raman spectrum shows the Hg‐Hg stretching vibration at 177 cm—1 within the Hg22+ ion additionally.  相似文献   

13.
(n)MnOx–(1?n)CeO2 binary oxides have been studied for the sorptive NO removal and subsequent reduction of NOx sorbed to N2 at low temperatures (≤150 °C). The solid solution with a fluorite-type structure was found to be effective for oxidative NO adsorption, which yielded nitrate (NO? 3) and/or nitrite (NO? 2) species on the surface depending on temperature, O2 concentration in the gas feed, and composition of the binary oxide (n). A surface reaction model was derived on the basis of XPS, TPD, and DRIFTS analyses. Redox of Mn accompanied by simultaneous oxygen equilibration between the surface and the gas phase promoted the oxidative NO adsorption. The reactivity of the adsorbed NOx toward H2 was examined for MnOx–CeO2 impregnated with Pd, which is known as a nonselective catalyst toward NO–H2 reaction in the presence of excess oxygen. The Pd/MnOx–CeO2 catalyst after saturated by the NO uptake could be regenerated by micropulse injections of H2 at 150 °C. Evidence was presented to show that the role of Pd is to generate reactive hydrogen atoms, which spillover onto the MnOx–CeO2 surface and reduce nitrite/nitrate adsorbing thereon. Because of the lower reducibility of nitrate and the competitive H2–O2 combustion, H2–NO reaction was suppressed to a certain extent in the presence of O2. Nevertheless, Pd/MnOx–CeO2 attained 65% NO-conversion in a steady stream of 0.08% NO, 2% H2, and 6% O2 in He at as low as 150 °C, compared to ca. 30% conversion for Pd/γ–Al2O3 at the same temperature. The combination of NOx-sorbing materials and H2-activation catalysts is expected to pave the way to development of novel NOx-sorbing catalysts for selective deNOx at very low temperatures.  相似文献   

14.
Microwaves applied to a pyrolytic carbon matrix enhance the chemical reactions of SO2 and NOx decomposition. The SO2 and NOx in a coal combustor product gas are adsorbed in a char bed and decomposed by the microwave to elemental sulfur and nitrogen, respectively. High removal rates of SO2 and NOx -- near 98% -- were observed in the laboratory tests. The activated carbon used as an adsorbent is also produced inexpensively in the electromagnetic field from coal pyrolysis. During the 21-cycle adsorption and decomposition experiments, the surface area of the bed carbon was increased from 7 m2/g to 700 m2/g. Process concept testing and economic evaluation will be completed in the U.S. Department of Energy, SBIR Phase II Program under Contract Number DE-FG03-90ER80898. This program is also supported in part by the National Science Foundation under Grant Number EHR-910-8774. The paper presents the laboratory test results obtained to date.  相似文献   

15.
Direct synthesis of nanosheet Fe-ZSM-5 catalysts and their use for selective catalytic reduction (SCR) of NO x by ammonia were studied. XRD, BET, SEM, EPR, and NH3-TPD were used to understand the properties of catalysts with different iron loading. XRD confirmed the presence of the ZSM-5 crystal phase, and there was no Fe2O3 phase on the surface of the crystals. SEM showed the Fe-ZSM-5 catalysts comprised microspheres made up of nanosheets. EPR indicated that the iron was present as isolated Fe3+and FeO x oligomers uniformly dispersed throughout the crystals. NH3-TPD indicated that Fe-ZSM-5 (20,1:1) had maximum acid sites and density at approximately 250 and 450 °C, respectively. Fe-ZSM-5 (20,1:1) had the highest activity in the SCR reaction with NH3. It was also confirmed that Fe-ZSM-5 (20,1:1) had excellent resistance to SO2 and H2O under the SCR reaction conditions. The effects of water vapor and SO2, iron loading, and the Si/(Fe + Al) ratio were also investigated for these catalysts.  相似文献   

16.
采用浸渍法和共沉淀法制备了Ho Ce Mn/Ti O2脱硝催化剂并对其结构和性能进行了表征。结果表明共沉淀法增强了活性组分和载体的相互作用,从而增加了Ho Ce Mn Ti-C催化剂表面Ce3+、Mn4+以及吸附氧的含量,使其表现出优异的低温氧化还原性能。此外,共沉淀法制备的HoCeMnTi-C具有更多的表面酸性位点及更强的表面酸性。催化剂表面酸性和氧化还原性能的提高有助于氨的吸附和活化,从而显著提高其活性。表面酸性位点的增多还抑制了H2O和SO2在催化剂表面的吸附,提升了催化剂的抗水抗硫性能。催化剂上的选择性催化还原(SCR)反应遵循Eley-Rideal(E-R)机制,催化剂硫中毒是源于形成的硫酸盐覆盖或破坏了催化剂活性位。  相似文献   

17.
A new ion chromatography method is described for the simultaneous determination of Cl, NO3 and SO42−, using a selected eluent 1.3-mM sodium gluconate/1.3-mM borax (pH 8.5). The extraction methods of Cl, NO3, SO42− in vegetables are studied. The determination limits of Cl, NO3, SO42− are 0.17 μg/ml, 0.63 μg/ml and 0.81 μg/ml. The linear ranges are 060 μg/ml, 090 μg/ml and 090 μg/ml. The relative S.D. are <2.5%. The mean recoveries of Cl, NO3, SO42− in vegetables range from 97.0 to 104%.  相似文献   

18.
Colourless needles of mercurous dimethylglyoximato nitrate, Hg2(Dmg)2(NO3)2, grow from a diluted nitric acid solution of mercurous nitrate and dimethylglyoxime. The crystal structure (triclinic, P1¯, a = 728.50(13), b = 1066.8(2), c = 1167.9(2) pm, α = 93.78(2)°, β = 94.16(2)°, γ = 98.61(2)°, Rall = 0, 0726) contains the cations [Hg2(Dmg)2]2+ and “non‐coordinating” (NO3) anions. In the cation, two neutral dimethylglyoxime molecules coordinate bidentately with Hg—N distances in the narrow range of 236 to 239 pm to the mercurous ion, Hg22+, which exhibits a Hg—Hg bond distance of 252.23(8) pm).  相似文献   

19.
Manganese‐ and cerium oxide‐modified titania catalysts were prepared by the deposition precipitation for the removal of elemental mercury (Hg0) from simulated yellow phosphorus off‐gas at low temperature. In addition, these catalysts were characterized by X‐ray diffraction, Brunauer–Emmett–Teller measurements, X‐ray photoelectron spectroscopy and field‐emission scanning electron microscope to determine the surface morphology of the obtained compounds and explore their formation mechanism. The results revealed that a Mn–Ce loading and reaction temperature of 10% and 150 °C, respectively, as well as a Mn/Ce molar ratio of 2:1, led to an optimal efficiency for the oxidation of elemental mercury. Furthermore, the effects of flue gas components were investigated. The presence of O2 clearly promoted the oxidation of Hg0. A CO atmosphere did not affect the Hg0 oxidation, when compared with N2, whereas the presence of H2S and water vapor inhibited the oxidation process. Furthermore, the X‐ray photoelectron spectroscopy spectra of Hg 4f revealed that the elemental mercury adsorbed by the catalyst is present as HgO. Finally, the Hg0 catalytic oxidation mechanism was discussed on the basis of the experimental results and characterization analysis.  相似文献   

20.
采用浸渍法和共沉淀法制备了HoCeMn/TiO2脱硝催化剂并对其结构和性能进行了表征。结果表明共沉淀法增强了活性组分和载体的相互作用,从而增加了 HoCeMnTi-C催化剂表面 Ce3+、Mn4+以及吸附氧的含量,使其表现出优异的低温氧化还原性能。此外,共沉淀法制备的HoCeMnTi-C具有更多的表面酸性位点及更强的表面酸性。催化剂表面酸性和氧化还原性能的提高有助于氨的吸附和活化,从而显著提高其活性。表面酸性位点的增多还抑制了 H2O和 SO2在催化剂表面的吸附,提升了催化剂的抗水抗硫性能。催化剂上的选择性催化还原(SCR)反应遵循Eley-Rideal(E-R)机制,催化剂硫中毒是源于形成的硫酸盐覆盖或破坏了催化剂活性位。  相似文献   

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