Temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust

In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust(ATD) has been investigated within a temperature range of 255–315 K using a Knudsen cell reactor. Combined with diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) experiment, it was found that acrylic acid could adsorb on ATD via surface OH groups and convert to carboxylate on the particle surface. The kinetics study suggests that the initial true uptake coefficient(γt) of acrylic acid on ATD decreases from(4.02 ± 0.12) × 10~(-5) to(1.73 ± 0.05) × 10~/(-5)with a temperature increase from 255 to315 K. According to the temperature dependence of uptake coefficients, the enthalpy(ΔH obs)and entropy(ΔS obs) of uptake processes were determined to be-(9.60 ± 0.38) KJ/mol and-(121.55 ± 1.33) J·K/mol, respectively. The activation energy for desorption(E des) was calculated to be(14.57 ± 0.60) KJ/mol. These results indicated that the heterogeneous uptake of acrylic acid on ATD surface was sensitive to temperature. The heterogeneous uptake on ATD could affect the concentration of acrylic acid in the atmosphere, especially at low temperature.     

La0.8Ca0.2FeO3/MgAl2O4丝网整体催化剂用于低浓度甲烷催化燃烧

开发了涂覆在金属丝网基体上的La_(0.8)Ca_(0.2)FeO_3/MgAl_2O_4复合整体催化剂,用于低浓度甲烷(0.5%,体积分数)催化燃烧反应.首先用沉积-沉淀法制备了La_(0.8)Ca_(0.2)FO_3(LCF)钙钛矿与Mg Al_2O_4尖晶石复合的粉末催化剂LCF/Mg Al2O4,用程序升温微反应器(TPRS)测定了粉末活性,结合XRD、BET、SEM、TPR的表征结果,筛选出了最佳复合物质的量比和最适焙烧温度.当LCF与Mg Al_2O_4复合后,抗烧结能力增强,以拟一级反应速率常数(k,L·g~(-1)·s~(-1))计的活性提高了1倍左右.然后采用浆料涂覆法,在表面改性的金属丝网蜂窝基体上分层涂覆了作为第二载体的MgAl_2O_4和LCF/Mg Al_2O_4复合粉体涂层,考察了复合粉体球磨前焙烧的温度、第二载体及活性层涂覆量的影响.最后在空速GHSV=40000 h~(-1)条件下测试了甲烷催化燃烧反应的活性.与陶瓷基体相比,涂覆在金属丝网基体上的LCF/MgAl_2O_4活性在600℃时提升了48.1%.500 h长运转试验发现,催化剂活性在初期的200 h下降了20.3%,然后基本保持稳定.     

Do aerosols act as catalysts in the OH radical initiated atmospheric oxidation of volatile organic compounds?

Smog chamber/FTIR techniques were used to study the relative reactivity of OH radicals with methanol, ethanol, phenol, C₂H₄, C₂H₂, and p-xylene in 750 Torr of air diluent at 296±2 K. Experiments were performed with, and without, 500–8000 μg m⁻³ (4000–50 000 μm² cm⁻³ surface area per volume) of NaCl, (NH₄)₂SO₄ or NH₄NO₃ aerosol. In contrast to the recent findings of Oh and Andino (Atmospheric Environment 34 (2000) 2901, 36 (2002) 149; International Journal of Chemical Kinetics 33 (2001) 422) there was no discernable effect of aerosol on the rate of loss of the organic compounds via reaction with OH radicals. Gas kinetic theory arguments cast doubt upon the findings of Oh and Andino. The available data suggest that the answer to the title question is “No”. As part of this work the rate constants for reactions of OH radicals with methanol, ethanol, and phenol in 750 Torr of air at 296 K were determined to be: k_OH+CH3OH=(8.12±0.54)×10⁻¹³, k_OH+C2H5OH=(3.47±0.32)×10⁻¹² and k_OH+phenol=(3.27±0.31)×10⁻¹¹ cm³ molecule⁻¹ s⁻¹.     

Removal of VOCs from gas streams with double perovskite-type catalysts

Double perovskite-type catalysts including La2 CoMnO_6 and La_2 CuMnO_6 are first evaluated for the effectiveness in removing volatile organic compounds(VOCs), and single perovskites(La CoO_3, LaMnO_3, and La Cu O3) are also tested for comparison. All perovskites are tested with the gas hourly space velocity(GHSV) of 30,000 hr~(-1), and the temperature range of100–600°C for C_7H_8 removal. Experimental results indicate that double perovskites have better activity if compared with single perovskites. Especially, toluene(C_7H_8) can be completely oxidized to CO_2 at 300°C as La2 Co MnO_6 is applied. Characterization of catalysts indicates that double perovskites own unique surface properties and are of higher amounts of lattice oxygen,leading to higher activity. Additionally, apparent activation energy of 68 k J/mol is calculated using Mars-van Krevelen model for C7 H8 oxidation with La2 Co Mn O6 as catalyst. For durability test, both La2 Co Mn O6 and La_2 CuMnO_6 maintain high C7 H8 removal efficiencies of 100% and98%, respectively, at 300°C and 30,000 hr~(-1), and they also show good resistance to CO_2(5%) and H2 O(g)(5%) of the gas streams tested. For various VOCs including isopropyl alcohol(C_3H_8 O),ethanal(C_2H_4O), and ethylene(C_2H_4) tested, as high as 100% efficiency could be achieved with double perovskite-type catalysts operated at 300–350°C, indicating that double perovskites are promising catalysts for VOCs removal.     

烟气脱硝装置与电厂设备运行的相互影响

火电厂烟气脱硝装置中的二氧化硫、灰分、氨及催化剂中的各种重金属在高温烟气的作用下发生各种化学作用,生成的硫酸氢氨等产物对火电厂的各种设备均会产生不同影响.同时由于系统阻力及荷载的变化,也会对电厂其他相关设备产生影响,根据目前工程的运行经验,火电厂在增设脱硝装置后,均会对空气预热器、引风机、锅炉钢架等进行改造.通过综合分析烟气脱硝装置产生的影响原因及解决办法,为脱硝装置的设计提供参考.     

La2O3—ZrO2缺陷萤石型燃烧催化剂的制备

缺陷萤石型Ｌａ２Ｏ３－ＺｒＯ２固溶体的催化燃烧活性受制备条件的影响，本文通过对其共沉淀前体的表面结构和热分解过程的分析，发现共沸蒸馏的办法可以有效地控制前体表面羟基的缩合过程，减少团聚，保持前体中金属离子均匀分散，为生成缺陷有序的烧结石型的Ｌａ２Ｚｒ２Ｏ７复氧化物提供了可能。复合氧化物固溶体的表面阳离子配置情况与样品的催化氧化性能密切相关，软团聚前体的烧结产物对甲烷燃烧反应具有更高的催化活性。     

TiO2催化超声降解月桂醇聚氧乙烯(9)醚溶液

表面活性剂随废水、废物的排放进入水体或土壤等环境,会对环境造成严重的污染.因此,有必要在其排放之前采用既安全可靠又有效的方法对其进行处理.本文采用经过600℃高温处理的锐钛矿型TiO2作为催化剂,以超声催化降解月桂醇聚氧乙烯(9)醚(AEO9)反应为模型,研究各种因素对TiO2催化超声降解的影响.结果表明,在TiO2催化剂作用下超声降解AEO9是可行的,且效果明显.在超声波功率为600 W,经600℃活化的TiO2催化剂用量为0.5～0.7g/L,AEO9水溶液初始质量浓度为60 mg/L,初始pH值为4.0的条件下,降解2 h后,AEO9降解率可达99%以上.     

非热等离子体结合CuO催化剂或Ca(OH)2吸收剂去除氮氧化物

采用非热等离子体结合催化或现场化学吸收的2种方法来去除气流中的NO_x.结果表明,非热等离子体结合催化,反应器内的CuO催化剂能有效地促进NO的还原反应;相对于催化还原NO而言,脉冲电晕作用下能有效地降低NO催化还原的反应温度.当催化剂为CuO,脉冲电压为18kV,反应温度为200℃,还原剂为1%CO及NO进口浓度为719 mg/m³条件下,NO的去除率达到了100%.非热等离子体结合现场化学吸收方法,是一种在常温下从气流中净化氮氧化物的有效方法,NO的去除率远远高于反应器内没有吸收剂的情况.可以认为反应器内的Ca(OH)₂吸收剂通过与NO的氧化产物NO₂或NO₃的吸收反应促进了NO的去除.当反应器内有Ca(OH)₂吸收剂存在时,在脉冲电压为18kV,O₂浓度为2%及NO进口浓度为1 050 mg/m³条件下,NO的去除率达到了100%.     

污泥热解催化剂的研究进展

污泥热解处理技术具有较好的应用价值和发展前景,催化剂的加入可提高反应效率,降低处理成本,提高目标产物品质。本文综述了添加不同种类污泥热解催化剂对反应条件、反应过程、反应产物的影响,分析了不同种类催化剂的优势与不足,并对该领域未来的研究方向提出了建议。指出:应深入探究催化剂的作用机理,开发高效、环保型催化剂;重点研发废弃物制备催化剂,实现废物资源化利用;开展污泥与其他废弃物共热解的研究。     

改性镍铝催化剂氧化零价汞及抗氨干扰机理

采用尿素水解法制备NiAlO和NiAlMO(M=Zn、Ba、Mn、La、Cr)催化剂用于Hg0催化氧化研究.结果表明,在NH3存在时,NiAlZnO催化剂展现出最好的Hg0氧化活性,250℃时Hg0的转化率超过80％,并在350℃达到最高(90％).Raman和XPS结果显示,Zn掺杂构成Ni-O-Zn固溶体,引起Ni...