以堇青石蜂窝陶瓷为载体的新型钒氧化物脱氮催化剂研究

以TiO₂/Al₂O₃/堇青石蜂窝陶瓷为载体,以V₂O₅-MoO₃-WO₃为活性组分,用于氨法选择性催化还原烟气中NO的新型催化剂,并对该催化剂的活性性能和微观结构进行了评价和表征.同时,将该催化剂的活性性能与其它几种活性组分相同但载体、制备方法、结构不同的催化剂进行了对比.对比结果表明,该新型催化剂能取得最好的选择性催化还原氮氧化物催化性能BET、FT IR、XPS表征实验结果表明,其高催化活性得益于大比表面积及大孔体积,而TiO₂/Al₂O₃/堇青石蜂窝陶瓷载体及其制备方法对获得好的催化剂构型起了至关重要的作用.     

蜂窝状Ce/Cr掺杂Cu基催化剂用于乙烷的催化燃烧

以蜂窝堇青石陶瓷为载体,采用浸渍法负载氧化铝涂层和活性组分,制备了蜂窝状Ce/Cr掺杂Cu基催化剂。运用BET,XRD,XPS,H₂-TPR技术对催化剂进行了表征,并对其乙烷催化燃烧活性进行了评价。表征结果显示,Ce/Cr掺杂提高了催化剂表面化学吸附氧的含量,提升了催化剂在较低温度下的氧化还原性能。实验结果表明：在入口乙烷质量浓度2 000 mg/m³、反应空速20 000 h^-1的条件下,Cu-Ce催化剂较Cu催化剂的T₅₀和T₉₀（乙烷转化率为50%和90%时的反应温度）分别降低了46 ℃和101 ℃,降幅高于Cu-Cr催化剂的38 ℃和78 ℃;较高反应空速（30 000 h^-1）对催化反应不利,乙烷浓度对催化剂活性的影响不明显;550 ℃下Cu-Ce催化剂对乙烷的转化率100 h内保持在99%以上,表现出良好的稳定性。     

Fe-Mn-sepiolite as an effective heterogeneous Fenton-like catalyst for the decolorization of reactive brilliant blue

A study of the decolorization of reactive brilliant blue in an aqueous solution using Fe-Mn-sepiolite as a heterogeneous Fenton-like catalyst has been performed. The Fourier transform infrared (FTIR) spectra of the catalyst showed bending vibrations of the Fe-O. The X-ray diffraction (XRD) patterns of the catalyst showed characteristic diffraction peaks of α-Fe₂O₃, γ-Fe₂O₃ and MnO. A four factor central composite design (CCD) coupled with response surface methodology (RSM) was applied to evaluate and optimize the important variables (catalyst addition, hydrogen peroxide dosage, initial pH value and initial dye concentration). When the reaction conditions were catalyst dosage= 0.4 g, [H₂O₂]= 0.3 mL, pH= 2.5, [reactive brilliant blue]_o = 50 mg·L⁻¹, and volume of solution= 500 mL at room temperature, the decolorization efficiency of reactive brilliant blue was 91.98% within 60 min. Moreover, the Fe-Mn-sepiolite catalyst had good stability for the degradation of reactive brilliant blue even after six cycles. Leaching of iron ions (<0.4 mg·L⁻¹) was observed. The decoloring process was reactive brilliant blue specific via a redox reaction. The benzene ring and naphthalene ring were first oxidized to open ring; these were then oxidized to the alcohol and carboxylic acid. The reactive brilliant blue was decomposed mainly by the attack of ·OH radicals including surface-bound ·OH radicals generated on the catalyst surface.     

Chemical poison and regeneration of SCR catalysts for NOx removal from stationary sources

Selective catalytic reduction (SCR) of NO_x with NH₃ is an effective technique to remove NO_x from stationary sources, such as coal-fired power plant and industrial boilers. Some of elements in the fly ash deactivate the catalyst due to strong chemisorptions on the active sites. The poisons may act by simply blocking active sites or alter the adsorption behaviors of reactants and products by an electronic interaction. This review is mainly focused on the chemical poisoning on V₂O₅-based catalysts, environmental-benign catalysts and low temperature catalysts. Several common poisons including alkali/alkaline earth metals, SO₂ and heavy metals etc. are referred and their poisoning mechanisms on catalysts are discussed. The regeneration methods of poisoned catalysts and the development of poison-resistance catalysts are also compared and analyzed. Finally, future research directions in developing poisoning resistance catalysts and facile efficient regeneration methods for SCR catalysts are proposed.     

复合金属氧化物Cu-Co-Al低温催化水解HCN

采用共沉淀法制备了Cu-Al、Co-Al和Cu-Co-Al复合金属氧化物催化剂,考察了3种催化剂对HCN的催化水解性能,并通过XRD、BET、XPS和H2-TPR等对催化剂的结构和性能进行表征.结果表明, Cu-Co-Al催化剂展示最高的催化活性. 反应温度200℃,反应180min后, Cu-Co-Al、Cu-Al和Co-Al催化剂对HCN的转化率分别为95%,90%,10%;NH3生成量分别为122,118,18mg/m3.低结晶度、高分散性、高比表面积的催化剂有利于低温HCN水解.适量的表面分子氧含量、较高的Cu2+和Co3+含量、较低的还原温度是Cu-Co-Al催化剂具有较高的HCN低温水解活性的主要原因.     

DOC+CDPF对生物柴油燃烧颗粒排放特性的影响

以一台满足国五排放法规的车用柴油机为样机,研究加装氧化催化转化器DOC与催化型颗粒捕集器CDPF(DOC+CDPF后处理装置)前后,柴油机燃用B20燃料(燃料含20%体积掺混比的生物柴油)的颗粒排放特性.结果表明,在未加装该后处理装置时,该机排气颗粒数量浓度的粒径分布呈双峰形态,B20燃料的排气颗粒数量浓度的峰值粒径在10nm和50nm附近,纯柴油的排气颗粒数量浓度的峰值粒径在50nm和200nm附近.在颗粒粒径小于120nm的区域,该机燃用B20燃料的排气颗粒数量浓度大于纯柴油.加装该后处理装置后,该机排气颗粒数量浓度的粒径分布呈多峰形态,峰值粒径在10nm、20nm和60nm附近.加装DOC+CDPF后,不论是柴油还是B20燃料,与原机相比,柴油机排气颗粒总数量下降明显,其中60~200nm粒径范围的颗粒数量浓度降幅更为显著.在相同工况下,DOC+CDPF对柴油机燃用B20燃料的颗粒总数量净化效率高于纯柴油.     

铁基催化剂的微波水热处理对其SCR脱硝性能的影响

利用微波对共沉淀制备的铁铈钛复合氧化物催化剂前驱体进行水热处理,探讨了微波水热处理对铁基催化剂低温SCR脱硝性能的优化;并对微波水热处理条件的影响进行了正交分析.结果表明:对铁基催化剂前驱体进行微波水热处理,可提高其低温SCR脱硝性能,使其脱硝温度窗口向低温偏移;且微波水热处理的低温优化效果与催化剂中Fe/Ti摩尔比密切相关,Fe/Ti摩尔比越小,微波水热处理的低温优化越强;微波加热方式和微波辐射时间会影响微波水热处理对铁基催化剂SCR脱硝性能的低温优化;在相同微波辐射时间条件下,当P30逐渐变为P80,微波水热处理对铁基催化剂低温SCR脱硝的促进作用降低;在P30条件下,微波辐射15min使铁基催化剂具有最佳低温SCR脱硝活性.     

贵金属-稀土复合型催化剂的制备与性能研究

制备了净化车辆尾气的贵金属稀土复合型催化剂,对该催化剂进行了活性测试和结构表征.利用所制备的催化剂在摩托车上进行了性能研究.实验结果表明,采用催化剂后,可使车辆排放达到欧洲Ⅱ号标准,表明所研制的催化剂具有较好的应用价值.     

Effects of a diesel oxidation catalyst on gaseous pollutants and fine particles from an engine operating on diesel and biodiesel

The effects of a diesel oxidation catalytic (DOC) converter on diesel engine emissions were investigated on a diesel bench at various loads for two steady-state speeds using diesel fuel and B20. The DOC was very effective in hydrocarbon (HC) and CO oxidation. Approximately 90%–95% reduction in CO and 36%–70% reduction in HC were realized using the DOC. Special attention was focused on the effects of the DOC on elemental carbon (EC) and organic carbon (OC) fractions in fine particles (PM_2.5) emitted from the diesel engine. The carbonaceous compositions of PM_2.5 were analyzed by the method of thermal/optical reflectance (TOR). The results showed that total carbon (TC), OC and EC emissions for PM_2.5 from diesel fuel were generally reduced by the DOC. For diesel fuel, TC emissions decreased 22%–32% after the DOC depending on operating modes. The decrease in TC was attributed to 35%–97% decrease in OC and 3%–65% decrease in EC emissions. At low load, a significant increase in the OC/EC ratio of PM_2.5 was observed after the DOC. The effect of the DOC on the carbonaceous compositions in PM_2.5 from B20 showed different trends compared to diesel fuel. At low load, a slight increase in EC emissions and a significant decrease in OC/EC ratio of PM_2.5 after DOC were observed for B20.     

UV185+254nm辐照下MnOx-TiO2分解甲醛与臭氧的机理

为提高185nm真空紫外光下甲醛与副产物臭氧的分解效率,以MnOx-TiO2复合催化剂取代TiO2光催化剂,发现甲醛与臭氧的转化率分别从44.7%和38.7%提高到77.5%和96.8%.研究比较了真空紫外光下和暗态下(加臭氧)甲醛与臭氧在MnOx-TiO2催化剂上的分解性能,及UV254nm下光催化分解甲醛的效率.结果表明,真空紫外光下气相活性氧物种的氧化与MnOx表面的臭氧催化氧化过程是甲醛分解的主要途径,而MnOx-TiO2上光催化氧化甲醛效率很低;副产物臭氧主要于MnOx表面活性位上由热催化分解.用真空紫外光辐照MnOx-TiO2催化剂,可提高MnOx催化分解臭氧的稳定性.