γ-Al_2O_3负载氧化锰催化臭氧化苯酚的研究

采用纳米级γ-Al_2O_3作为催化剂基体,制备γ-Al_2O_3负载氧化锰纳米催化剂来催化臭氧化降解水中的苯酚。采用浸渍法制备负载型的金属氧化物催化剂,以间歇反应的方式对不同浸渍浓度下催化剂的效能,不同催化剂投加量及苯酚溶液初始pH值等影响因素进行了深入研究。研究表明,4%Mn/γ-Al_2O_3催化剂显著提高了臭氧化降解水中苯酚的效果。催化剂投加量试验研究表明4%Mn/γ-Al_2O_3催化剂具有更多的活性位点。基于此,提出了催化臭氧化苯酚的反应机理。     

负载型湿式氧化催化剂RuO2/γ-Al2O3活性与稳定性

采用浸渍法制备了RuO2 /γ Al2 O3 催化剂 ,以苯酚为目标有机物重点研究了进水 pH值和温度对RuO2 /γ Al2 O3 催化剂组分溶出和活性的影响 .结果表明 ,催化剂在降解苯酚过程中存在着组分溶出现象 ,随着进水溶液pH值降低催化剂组分溶出量增加 ,且在进水为酸性时苯酚去除率高于碱性时的去除率 .反应温度升高 ,催化剂组分溶出量降低 ,苯酚去除率增加 .采用在负载型RuO2 /γ Al2 O3 催化剂中掺杂Ce和Zr的方法对抑制催化剂组分溶出进行了初步研究 ,发现掺杂Ce和Zr后有效地降低了RuO2 /γ Al2 O3 催化剂组分的溶出 ,且提高了催化剂的活性     

CeFeMn@ZSM-5催化臭氧氧化苯酚废水

采用等体积浸渍法制备新型CeFeMn@ZSM-5复合催化剂。以模拟苯酚废水COD去除率为主要考察指标,通过单因素条件实验,考察并确定催化降解苯酚废水较适宜的工艺条件为：活性组分负载量10%、废水初始pH=7,催化剂投加量6 g·L^-1。此条件下反应30 min,苯酚废水的COD去除率可达71.03%。催化剂重复使用实验结果显示,所制备的复合催化剂具有较高的稳定性和可重复使用性。     

催化臭氧氧化活性艳红X-3B水溶液中催化剂的研制

以金属Ni、Co为活性组分、γ-Al2O3为载体,用浸渍法制备催化剂催化臭氧氧化法处理活性艳红X-3B废水,并通过:XRD,SEM等检测手段进行表征.考察了浸溃时间、Ni占负载活性组分的摩尔比、焙烧温度和焙烧时间对催化活性的影响.结果表明:浸渍时间为8.5小时、镍占负载活性组分的摩尔比为0.67、焙烧温度为300℃、焙烧时间为5小时时制备的催化剂效果最佳.     

黏土负载型类Fenton催化剂的研究进展

黏土负载型类Fenton催化剂是将活性金属固定在黏土上,用以催化活化H₂O₂产生羟基自由基去除难降解有机污染物,克服了均相Fenton氧化适用pH范围窄、易产生铁泥沉淀等缺点。本文从黏土的类型和结构特点出发,简述了层状与非层状黏土负载活性金属的特点及其催化性能;分析了柱撑、浸渍、沉积-沉淀等活性金属负载方法和黏土的改性手段;阐述了负载活性金属类型及其对催化性能的影响。针对黏土负载型类Fenton催化剂的特点和现阶段存在的问题,从黏土负载型催化剂的活性金属负载形式、负载方法和高效稳定催化性能的需求等角度指出了今后的研究方向。     

金属负载型有序介孔碳催化剂的制备及应用研究进展

在金属负载型有序介孔碳催化剂的制备工艺过程中,合成比表面积高、孔道结构规整、活性组分高度分散以及粒径尺寸小的催化剂是当前研究的热点,常用的制备方法有浸渍法、化学还原法、一步合成法及共组装合成法等。通过对介孔碳载体改性并采用不同的制备方法调控活性金属在有序介孔碳载体中的粒径及分散度,可提高其在工业废水处理、电化学、催化、储氢等领域的性能。     

脂肪腈加氢制备单烷基二甲基叔胺催化剂的研究

通过对催化剂活性组分的筛选,钯/碳(Pd/C)催化剂对脂肪腈与二甲胺反应制备单烷基二甲基叔胺有良好的选择性。采用浸渍-沉淀法制备出负载型Pd/C催化剂,考察了制备过程中溶液体系的pH值和浸渍时间对Pd/C催化剂性能的影响。结果表明:该溶液体系在pH值7.9和浸渍15 h~18 h的条件下得到的Pd/C催化剂对脂肪腈催化加氢制备单烷基二甲基叔胺有较好的催化性能。     

负载型金属催化剂制备新技术研究进展

负载型金属催化剂因为其独特的催化性能在众多领域得到广泛应用。传统的催化剂制备方法有浸渍法,沉淀法,离子交换法和熔融法等。文章综述了溶剂化金属原子浸渍法,超临界技术和微波技术在负载型金属催化剂制备中的应用。     

负载型湿式氧化催化剂RuO2/γ-Al2O3活性与稳定性

采用浸渍法制备了RuO₂/γ-Al₂O₃催化剂，以苯酚为目标有机物重点研究了进水pH值和温度对RuO₂/γ-Al₂O₃催化剂组分溶出和活性的影响.结果表明，催化剂在降解苯酚过程中存在着组分溶出现象，随着进水溶液pH值降低催化剂组分溶出量增加，且在进水为酸性时苯酚去除率高于碱性时的去除率.反应温度升高，催化剂组分溶出量降低，苯酚去除率增加.采用在负载型RuO₂/γ-Al₂O₃催化剂中掺杂Ce和Zr的方法对抑制催化剂组分溶出进行了初步研究，发现掺杂Ce和Zr后有效地降低了RuO₂/γ-Al₂O₃催化剂组分的溶出，且提高了催化剂的活性.     

金属负载沸石催化氧化苯酚的研究

本文采用浸渍法制备得到一系列过渡金属(Fe、Cu、Mn等)负载的改性沸石(ZSM-5)催化剂,并以苯酚为目标污染物,考察溶液初始pH值、苯酚初始浓度、催化剂投加量、H_2O_2投加量等因素对催化降解苯酚效果的影响。Fe-Mn-Cu-ZSM-5催化剂在pH=2-8范围内均能高效催化氧化苯酚废水。处理浓度为100 mg·L~(-1)的苯酚时,加入1 m L/L 30%H_2O_2和2g/L Fe-Mn-Cu-ZSM-5催化剂,在紫外光照下反应60 min,其苯酚去除率大于90%。通过分析Fe-Cu-Mn-ZSM-5催化氧化苯酚的UV-VIS谱图和参考有关的文献,推断其反应机理为羟基自由基机理和光生空穴氧化机理的结合。     

Hydrogenation of carbon dioxide over metal catalysts prepared using microemulsion

This paper relates to a novel preparation method of metal supported catalysts using microemulsions. The size distribution of metal particles in the catalysts, thus, prepared was appreciably narrow and the average particle size was much smaller than that of the conventional catalyst prepared from impregnation. It was found that the particle size could be controlled by the conditions of microemulsions regardless of metal content. The Rh, Pd and Pt catalysts prepared from microemulsions were found to exhibit a much higher activity for the hydrogenation of carbon dioxide than those from impregnation.     

A comparative study of supported MoO3 catalysts prepared by the new “slurry” impregnation method and by the conventional method: their activity in transesterification of dimethyl oxalate and phenol

A new preparation method for supported MoO₃ catalyst, slurry impregnation, has been described and compared with the conventional impregnation method. Slurry MoO₃/water is used instead of the solution ammonium heptamolybdate, AHM [(NH₄)₆Mo₇O₂₄]. The MoO₃/γ-alumina, MoO₃/active carbon, and MoO₃/silica catalysts with different Mo loadings were prepared by slurry and by conventional method. The low solubility of MoO₃ was sufficient to transport molybdenum species from solid MoO₃ to the adsorbed phase. The equilibrium was achieved after several hours at 95 °C based on the loading amount of molybdenum. Only the process of drying was needed; calcination was not necessary and was left out. This is an important advantage for active carbon support because oxidative degradation of active carbon impregnated by molybdena starts at a relatively low temperature of about 250 °C during calcination on air. The activity was tested in the transesterification of dimethyl oxalate (DMO) and phenol at 180 °C. The dependences of catalytic activity on Mo loadings for the slurry prepared catalysts were similar to the dependences for the samples prepared by the conventional impregnation method with AHM. The activities of the slurry impregnation MoO₃/γ-Al₂O₃ catalysts were almost the same as those of catalysts prepared conventionally. Although the performances of slurry impregnation MoO₃/SiO₂ catalysts for transesterification of DMO were slightly better than those of the corresponding catalysts prepared by conventional impregnation, no waste solution and no calcining nitrogenous gases were produced. Therefore, we conclude that the new slurry impregnation method for preparation of supported molybdenum catalysts is an environmentally friendly process and a simple, clean alternative to the conventional preparation using solutions of (NH₄)₆Mo₇O₂₄. The present work will lead to a remarkable improvement in the catalyst preparation for the transesterification reaction.     

非均相微波协同类Fenton催化降解废水中的苯酚

通过等体积浸渍法制备了CuO/γ-Al_2O_3催化剂,并对非均相微波协同类Fenton催化降解苯酚溶液进行了实验研究。实验结果表明,在溶液初始pH为6,H_2O_2投加量为4 m L/L,催化剂投加量为4 g/L,微波功率为500 W,反应时间为13 min的条件下,苯酚降解率可达98%,TOC去除率为62%。催化剂重复使用9次后,苯酚降解率为90.88%。通过比较不同氧化体系处理效果及添加·OH捕获剂证实,微波-催化剂-H_2O_2产生了明显的协同作用。     

High activity PtRu/C catalysts synthesized by a modified impregnation method for methanol electro-oxidation

A modified impregnation method was used to prepare highly dispersive carbon-supported PtRu catalyst (PtRu/C). Two modifications to the conventional impregnation method were performed: one was to precipitate the precursors ((NH₄)₂PtCl₆ and Ru(OH)₃) on the carbon support before metal reduction; the other was to add a buffer into the synthetic solution to stabilize the pH. The prepared catalyst showed a much higher activity for methanol electro-oxidation than a catalyst prepared by the conventional impregnation method, even higher than that of current commercially available, state-of-the-art catalysts. The morphology of the prepared catalyst was characterized using TEM and XRD measurements to determine particle sizes, alloying degree, and lattice parameters. Electrochemical methods were also used to ascertain the electrochemical active surface area and the specific activity of the catalyst. Based on XPS measurements, the high activity of this catalyst was found to originate from both metallic Ru (Ru⁰) and hydrous ruthenium oxides (RuO_xH_y) species on the catalyst surface. However, RuO_xH_y was found to be more active than metallic Ru. In addition, the anhydrous ruthenium oxide (RuO₂) species on the catalyst surface was found to be less active.     

菲加氢裂化催化剂的初步研究

菲是一种稠环芳烃,存在于煤焦油中。在氢气存在的条件下,它可以在具有加氢和裂化活性的双功能催化剂上发生加氢裂化反应,该反应的关键就在于高性能催化剂的制备。采用浸渍法在不同条件下制备了Ni／Hβ催化剂,通过XRD和BET考察了负载量、浸渍时间、焙烧温度、焙烧时间对催化剂性能的影响,探讨最佳的制备条件及第一种金属的负载量,为双功能催化剂的制备提供实验依据和理论指导。     

Preparation,characterization and kinetic behavior of supported copper oxide catalysts on almond shell-based activated carbon for oxidation of toluene in air

Dispersed copper oxide nano-catalysts supported on almond shell-based activated carbon were prepared for catalytic oxidation of toluene in air. The response surface methodology was used to express the catalyst removal efficiency in terms of catalyst metal loading and calcination temperature. Catalyst activity increased with both increasing calcination temperature and metal loading. Calcination temperature had a significant effect on the catalyst activity only at high metal loadings. Two different catalyst preparation methods were employed to investigate the effect of impregnation technique on the deposition–precipitation method. Well-dispersed nano catalysts with higher efficiency towards oxidation of toluene were prepared by the heterogeneous deposition–precipitation (HDP) as compared with the combined impregnation and deposition–precipitation method. The support and catalyst properties were determined by X-ray diffraction, Transmission electron microscopy, field-emission scanning electron microscope, Boehm test, Brunauer–Emmett–Teller surface area measurements, and energy-dispersive X-ray spectroscopy. Characterization analyses and reaction experiments indicated the antonym effect of impregnation method on the deposition–precipitation method for catalyst preparation. Two types of crystallite (large and small) were formed on the support as a consequence of using the combined catalyst preparation method. Kinetic models were proposed for oxidation of toluene using copper oxide catalysts prepared by the HDP method. The kinetic study indicated that an Eley–Rideal mechanism could adequately describe the kinetic behavior of toluene oxidation.     

Highly reproducible syntheses of active Au/TiO2 catalysts for CO oxidation by deposition–precipitation or impregnation

Gold catalysts supported on TiO₂ were prepared by a deposition–precipitation (DP) method to investigate how highly reproducible performance of the gold catalysts in CO oxidation can be achieved. A protocol was established for synthesizing identically performing catalysts by different operators. The results show that for this synthesis route, the calcination step is not needed to form highly active Au/TiO₂ catalysts, but leads to decreased activity. Improved catalytic activity was observed when a high solution pH was adjusted during the precipitation. Surprisingly, wet impregnation followed by ammonia steam treatment and a washing step with water also leads to Au/TiO₂ with 2- to 4-nm individual gold particles highly dispersed on the TiO₂ surface. In addition, this catalyst is active for room temperature CO oxidation. The temperature for 50% conversion of CO is below 25 °C, which is comparable to that of the gold catalyst prepared by the DP method. Therefore, contrary to reports in the literature, the impregnation method can be used in the preparation of high-activity gold catalysts.     

A new and direct preparation method of iron-based bimodal catalyst and its application in Fischer–Tropsch synthesis

A bimodal iron-based catalyst was prepared by a new one-step impregnation method. The active components were used as the “brick” to directly build the small pores inside the large pores of support, which was quite different from the previous bimodal catalysts that were prepared once more on a bimodal support. Comparing with the unimodal catalysts and conventional co-precipitated catalyst, the prepared bimodal catalyst exhibited excellent activity in Fischer–Tropsch synthesis due to the improved active metal dispersion and fastened diffusion efficiency. This preparation method is much simpler than the previous methods and can be extended to prepare various bimodal catalysts with different chemical compositions.     

合成氯乙烯低汞催化剂制备

采用不同工艺条件制备氯乙烯低汞催化剂,利用固定床反应器对催化剂进行活性评价,筛选转化率和选择性较高的催化剂制备条件。结果表明,与等体积浸渍法相比,由于过饱和浸渍法制得的催化剂负载更多的Hg Cl2,在反应前期,催化剂活性较低,随着反应时间的延长,催化剂被完全激活,活性超过等体积浸渍法制备的催化剂。浸渍时间、水浴温度和溶液p H均影响活性炭对Hg Cl2的吸附量,在浸渍时间6 h、水浴温度60℃和p H=1条件下,控制Hg Cl2质量分数为5.35%,120℃干燥20 h制备的催化剂具有较理想的活性。复合助剂的加入有助于提高催化剂活性与热稳定性,当n(Hg Cl2)∶n(Ce Cl3)∶n(KCl)=1∶1∶1时拥有更高活性,添加更多助剂堵塞活性炭孔道,降低催化剂活性。