催化氧化NO催化剂Mn/ZrO2的制备与性能研究

以二氧化锆为载体负载锰氧化物,制备了MnO x/ZrO2催化剂用于催化氧化法(SCO)脱除烟气NO,考察了制备条件和反应条件对催化剂SCO活性的影响.同时,采用N2吸附、SEM、XRD及XPS等手段对催化剂理化性质进行了表征.结果表明,采用等体积浸渍法,以硝酸锰作为前驱体制备的Mn8/ZrO2/450催化剂在300℃、空速15000 h-1条件下,NO转化率可达84%,表现出较好的NO氧化活性.催化剂的主要活性组分为MnO2,在催化剂载体表面上呈现出较好的分散度.对催化剂进行了NO等温吸附与程序升温脱附,结合程序升温表面反应(TPSR)实验,探讨了催化剂表面NO催化氧化机理.研究发现,NO在该催化剂表面主要以吸附态反应,在含氧气氛中吸附态NO的氧化速率高于脱附速率,表面NO2的脱附峰温与最佳SCO活性温度相吻合.上述结果表明,NO转化过程速率受氧化产物NO2的脱附步骤控制,表面反应为快速步骤.     

多相催化臭氧氧化技术机理研究进展

多相催化臭氧氧化技术能够有效去除水中的微量有机物。尽管有越来越多的研究致力于多相催化臭氧氧化技术领域,以及各种新的催化剂的引入,但对于多相催化臭氧氧化技术机理尚不清楚。因此,本文针对多相催化臭氧氧化技术中常用的负载型金属、负载型金属氧化物以及活性炭三类催化剂的反应机理进行了探讨。此外还对机理研究中存在的问题进行了探讨。     

Oxidation of Toluene on γ-Al2O3 Supported Copper–Manganese Catalysts

Abstract Catalytic incineration of toluene over γ-Al2O3-supported copper–manganese oxide catalysts in the temperature range of 433?K–553?K was investigated using a fixed-bed flow reactor. Catalysts were characterized using Brunauer-Emmett-Teller surface area analysis, scanning electron microscopy, temperature-programmed reduction, temperature-programmed oxidation, X-ray photoelectron spectroscopy, and X-ray diffraction. Incineration of toluene was achieved at temperatures up to 553?K and it was found that the weight ratio of reactants (Cu:Mn) was optimized to be 15:10. Brunauer-Emmett-Teller surface area results had no correlation with the activity of the catalysts. Results of temperature-programmed reduction/temperature-programmed oxidation and X-ray photoelectron spectroscopy showed that the redox peak of the 15Cu-10Mn catalyst shifted at lower temperatures and the binding energy shifted toward higher oxidation levels. These results show that high binding energy and high redox capacity are the causes of...     

Study on catalysts for combustion of lean CH_4

ＳｔｕｄｙｏｎｃａｔａｌｙｓｔｓｆｏｒｃｏｍｂｕｓｔｉｏｎｏｆｌｅａｎＣＨ＿４ＺｈｏｕＺｅｘｉｎｇ，ＹｉｎＬｉｎｇ，ＸｕＪｉｎｇＫｅｓｅａｒｃｈＣｅｎｔｅｒｆｏｒＥｃｏ－ＦｎｖｉｒｏｎｍｅｎｔａｌＳｃｉｅｎｃｅｓ，ＣｈｉｎｅｓｅＡｃａｄｅｍｙｏｆＳｃ...     

过渡金属改性的Cr-Ce-O催化剂氧化氯苯性能

以氯苯为含氯挥发性有机污染物探针物,以稀土基CeO₂为基底活性氧化物,采用柠檬酸络合法制备Cr-Ce-O催化剂,考察Cr/Ce物质的量比、过渡金属氧化物掺杂及掺杂量、载体和焙烧温度对Cr-Ce-O催化剂催化氧化氯苯性能的影响;采用XRD、BET、SEM、H₂-TPR、XPS等表征技术分析催化剂的基本特性.研究表明,Cr₂O₃和CeO₂间形成了CrCeO_x固溶体,掺杂有ZrO₂的Cr₂O₃-CeO₂/Al₂O₃催化剂其比表面积得到显著提升,且载体对催化剂活性组分形态结构产生重要影响,其中以焙烧温度为400℃,堇青石为载体的催化剂氧化活性较优.研究发现,ZrO₂掺杂量亦对催化剂氧化活性产生显著性影响,当Zr/Cr物质的量比为1：2时,Cr₂O₃-CeO₂-ZrO₂/堇青石催化剂表现最佳,催化氧化氯苯转化率可达92.7%（反应温度为350℃）,这主要是由于ZrO₂掺入促进了CeO₂和Ce₂O₃,Cr₂O₃和ZrO₂间的相互作用,氧空位增加促使表面活性氧（O_sur）增多.     

PM-support interfacial effect and oxygen mobility in Pt,Pd or Rh-loaded (Ce,Zr,La)O2 catalysts

• Pt/CZL exhibits the optimum catalytic performance for HC and NO_x elimination. • The strong PM-Ce interaction favors the oxygen mobility and DOSC. • Pd/CZL shows higher catalytic activity for CO conversion due to more O_latt species. • Great oxygen mobility at high temperature broadens the dynamic operation window. • The relationship between DOSC and catalytic performance is revealed. The physicochemical properties of Pt-, Pd- and Rh- loaded (Ce,Zr,La)O₂ (shorted for CZL) catalysts before/after aging treatment were systematically characterized by various techniques to illustrate the relationship of the dynamic oxygen storage/release capacity and redox ability with their catalytic performances for HC, NO_x and CO conversions. Pt/CZL catalyst exhibits the optimum catalytic performance for HC and NO_x elimination, which mainly contribute to its excellent redox ability and dynamic oxygen storage/release capacity (DOSC) at lower temperature due to the stronger PM (precious metals)-support interaction. However, the worse stability of Pt-O-Ce species and volatile Pt oxides easily result in the dramatical decline in catalytic activity after aging. Pd/CZL shows higher catalytic activity for CO conversion by reason of more O_latt species as the active oxygen for CO oxidation reaction. Rh/CZL catalyst displays the widest dynamic operation window for NO_x elimination as a result of greater oxygen mobility at high temperature, and the ability to retain more Rh-O-Ce species after calcined at 1100°C effectively restrains sintering of active RhO_x species, improving the thermal stability of Rh/CZL catalyst.     

废旧车用载钯催化剂中钯的浸出研究

针对汽车尾气的污染,汽车排气系统都安装有含铂族金属的汽车催化剂.废旧汽车催化剂已成为铂族金属重要的二次资源.本文采用湿法浸出整体式蜂窝陶瓷汽车催化剂中的铂族金属钯.氧化焙烧废汽车催化剂除去积炭和其他有机物,再磨细过筛100目后烘干.预处理过的废催化剂用还原剂HCOOH溶液将催化剂中氧化态钯转化为单质钯,在70℃恒温下,用盐酸和氧化剂NaClO3选择性浸出钯.本文比较了几种浸出方法的结果,考察了HCl-NaClO3浸出体系的几个因素对钯浸出的影响,确定了最佳浸出条件.实验结果表明,HCl-NaClO3浸出体系在优化条件下能完全浸出催化剂中的钯,该方法可以用于钯的回收和对催化剂中的钯进行定量分析.     

催化超临界水氧化技术处理香料废水研究

采用催化超临界水氧化(CSCWO)技术对香料废水进行氧化处理,研究了催化剂浓度、反应温度、压力、停留时间等因素对废水COD、TN去除效果的影响.结果表明:在超临界水中添加cu2+催化剂后有机物的去除效率与无催化剂时相比有显著的提高.香料废水中COD、TN的去除率随催化剂浓度、反应温度和压力的升高,停留时间的延长而提高....     

Reduction of NO by CO using Pd-CeTb and Pd-CeZr catalysts supported on SiO2 and La2O3-Al2O3

The catalytic activity of Pd catalysts supported on Ce_0.73Tb_0.27O_x/SiO₂, Ce_0.6Zr_0.4O_x/SiO₂, Ce_0.73Tb_0.27O_x/La₂O₃-Al₂O₃ and Ce_0.6Zr_0.4O_x/La₂O₃-Al₂O₃ was studied using the reduction of NO by CO. The catalysts were characterized by X-ray fluorescence, surface area, X-ray diffraction, temperature-programmed reduction, CO chemisorption and oxygen storage capacity. Temperature-programmed reduction results indicated that Tb or Zr incorporation improves the reducibility and oxygen storage capacity. CO chemisorption data suggested the presence of large PdO particles due to the low CO/Pd ratio. No significant differences were obtained in light off temperatures (T_{Light off}) for all Pd catalysts and the most active was 1.5%Pd/Ce_0.6Zr_0.4O_x/SiO₂.     

Effect of water vapor on NH3-NO/NO2 SCR performance of fresh and aged MnOx-NbOx-CeO2 catalysts

A MnOx–NbOx–CeO2 catalyst for low temperature selective catalytic reduction(SCR) of NOx with NH3 was prepared by a sol–gel method, and characterized by NH3–NO/NO2 SCR catalytic activity, NO/NH3 oxidation activity, NOx/NH3 TPD, XRD, BET, H2-TPR and in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy(DRIFTS). The results indicate that the Mn Ox–Nb Ox–CeO2 catalyst shows excellent low temperature NH3-SCR activity in the temperature range of 150–300℃. Water vapor inhibits the low temperature activity of the catalyst in standard SCR due to the inhibition of NOx adsorption. As the NO2 content increases in the feed, water vapor does not affect the activity in NO2 SCR. Meanwhile, water vapor significantly enhances the N2 selectivity of the fresh and the aged catalysts due to its inhibition of the decomposition of NH4NO3 into N2O.