Au/α-Fe2O3催化剂选择性氧化富氢气中CO的性能研究

通过并流共沉淀法制备了Au/-Fe2O3催化剂,考察了金负载量及焙烧温度对Au/-Fe2O3催化剂的物化结构及其选择性氧化富氢气体中CO催化性能的影响。研究结果表明,金负载量和焙烧温度对催化剂的性能均有较大影响,金负载量为1.5%(wt),低温焙烧(200~400℃)时制得的Au/-Fe2O3催化剂对CO选择性氧化反应具有很好的催化活性和选择性,其中金负载量为1.5%(wt)、300℃焙烧的Au/-Fe2O3催化剂,在40℃时对富氢气体中CO的转化率达到100%,选择性为 66%,该催化剂连续反应120h催化活性没有明显下降。XRD、BET和TEM分析结果表明,催化剂的性能与单质Au的粒径有关,粒径越小,催化活性越高。     

甲醇水蒸汽重整制氢Au/TiO2催化剂

采用沉积-沉淀法制备了一系列Au/TiO2催化剂,考察了Au负载量、焙烧温度以及助剂等因素对甲醇水蒸汽重整制氢反应催化性能的影响;并利用XRD, TEM对催化剂进行了表征. 结果表明,制备条件对催化性能有明显影响;Au负载量为5%(w)时所得催化剂活性较好;助剂NiO可使催化剂催化甲醇水重整的催化活性明显提高;100℃烘干未焙烧制得的催化剂活性最好;TEM结果显示,NiO的加入使载体TiO2颗粒分散度提高,Au粒粒度变小.     

Au/TiO_2-B催化剂的CO低温氧化性能

探索Au纳米粒子对新型材料的催化性能可以显著拓宽金催化剂的应用范围。使用TiO2-B作为载体,担载Au纳米粒子并应用于低温CO氧化反应体系。TiO2-B为长度5~20?m的微米级纤维,Au纳米粒子粒径在3 nm以下,均匀地分散在TiO2-B表面。CO氧化测试表明,Au纳米粒子的性能受TiO2-B焙烧温度的影响,不同焙烧温度会引起Au分散性以及Au纳米粒子与载体相互作用的改变。分散于纯TiO2-B载体上的金的催化活性可与其分散在锐钛矿纳米粉体上的相媲美。此外,300℃下活化的Au纳米粒子表现出了最佳的CO氧化性能,在氧化性气氛中活化的催化剂的催化性能优于在惰性和还原性气氛中活化的催化剂。     

金掺杂TiO2纳米管的制备及其低温CO氧化催化性能

在NaOH溶液中水热处理TiO2粉末得到高比表面积的TiO2纳米管,通过浸渍-沉积法制备金掺杂TiO2纳米管(Au/TiO2 NTs).通过BET、XRD和TEM等手段对所得材料进行表征,并测定Au/TiO2 Nts对CO氧化的催化性能.载体的形态、制备过程中HAuCl4溶液的pH值、灼烧温度以及气氛、金含量对Au/TiO2 NTs的活性影响极大.     

Au/CeO_2-cube催化1,3-丙二醇氧化酯化反应性能

采用沉积-沉淀法制备了高活性的Au/Ce O2-cube催化剂,并对催化剂进行了电感耦合等离子发射光谱、透射电镜、X射线衍射和X射线光电子能谱表征。将制得的催化剂用于1,3-丙二醇选择性氧化酯化反应,考察了沉淀剂尿素的用量、Ce O2-cube载体焙烧温度、催化剂焙烧温度、Au负载量和沉积温度对反应性能的影响,结果表明:尿素和Ce O2-cube的质量比为6、沉积温度80℃、Ce O2-cube焙烧温度400℃、催化剂焙烧温度200℃制备的1.5%Au/Ce O2-cube,具有最优的催化活性。在100℃、O2分压2 MPa、1,3-丙二醇和Au的物质的量比为75.5的条件下反应4 h,1,3-丙二醇的转化率达到97.5%,3-羟基丙酸甲酯和丙二酸二甲酯的选择性分别达到90.1%和6.1%。将用过的催化剂在200℃焙烧2 h烧掉表面的中毒物质后循环使用4次,催化性能略有降低,性能下降主要是由催化反应过程中Au颗粒粒径的长大造成的;催化剂上2.0~4.0 nm左右的具有少量Auδ+的负载纳米Au单质颗粒有助于醇的氧化酯化反应。     

CuCoOx/TiO2催化氧化CO性能

采用浸渍法制备了CuCoOx/TiO2催化剂,并用XRD、TPR和BET进行了表征。350 ℃焙烧的催化剂CuCoOx/TiO2具有CuCo2O4尖晶石结构,比表面积大,对CO的催化氧化效果好,在110 ℃时可将1%的CO完全氧化成CO2。考察了催化剂焙烧温度、反应温度、CO进口浓度、空速对催化剂催化氧化CO性能的影响。该CuCoOx/TiO2催化剂具有良好的单独抗水和抗硫性能,可用于不同时存在二氧化硫和水的废气脱除CO。     

Au改性La0.8Sr0.2MnO3催化剂的催化燃烧性能

采用共沉淀（CP）和沉积-沉淀法（DP）分别制备了0.5%(质量分数)金掺杂的Au-LSM和Au/LSM钙钛矿催化剂,以甲苯催化燃烧为模型反应测试催化剂活性,并用XRD、BET、H₂-TPR对其进行表征。结果表明,Au掺杂并不改变La_0.8Sr_0.2MnO₃催化剂的织构性质,但明显增强了催化剂表面氧的活动性,提高了其低温催化氧化活性。与DP法制备的Au/LSM相比,Au-LSM表现出更好的催化性能,其催化活性与商业贵金属Pd/Al₂O₃相当。通过对焙烧温度考察以及50 h的变温活性测试,Au-LSM催化性能并没有发生较大变化,催化剂具有良好的稳定性。     

Au掺杂水热均匀沉淀高温制备TiO_2的光催化性能

向水热均匀沉淀、800℃焙烧制得的高活性、易分离TiO2(TiO2-800)中掺杂金(Au),以光催化降解活性艳红染料X-3B作为模型反应,考察了掺Au量、制备条件、Au的价态等对Au/TiO2-800光催化性能的影响。结果表明,氨水作为沉淀剂,200℃焙烧的0.5%Au/TiO2-800的光催活性较TiO2-800有较大提高,染料X-3B的降解率由93%提高到了100%。还原实验显示,0.5%Au/TiO2-800表面存在的离子态Au能有效提高TiO2-800光催化活性。     

纳米金催化剂室温下对甲醛的催化氧化

Fe Ox和Ce O2对于Au/Al_2O_3催化剂催化氧化甲醛是一种有效助剂。本文采用等体积浸渍法制备了Au/Fe Ox/Al_2O_3和Au/Fe Ox-Ce O2/Al_2O_3复合催化剂。考察金负载量和Fe Ox-Ce O2复合助剂对催化剂室温催化氧化甲醛的影响,并利用XRD、BET和透射电镜(TEM)对催化剂进行技术表征。研究表明:在Au负载量等同时,催化活性顺序是:Au/Fe O_x-Ce O_2/Al_2O_3Au/Fe O_x/Al_2O_3Au/Ce O2/Al_2O_3;Au负载量越高催化剂催化活性越好。     

氧化铬催化剂上NO常温催化氧化反应的性能研究

采用沉淀方法制备了氧化铬催化剂,并用于NO催化氧化反应,首次发现该催化剂具有常温氧化活性,考察了沉淀剂和焙烧温度等制备条件对其活性的影响。结果发现,相比于常规的活性炭及活性炭纤维,氧化铬催化剂在常温催化氧化NO方面表现出了更加优异的活性及稳定性,当NO质量分数为15μg/g,空速为43 200 m L/h时,可维持800 min以上100%净化率,采用氨水、碳酸氢铵、氢氧化钾作为沉淀剂时,300℃焙烧得到的氧化铬催化剂具有很好的活性及稳定性。     

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.     

Comparative study of Au/ZrO2 catalysts in CO oxidation and 1,3-butadiene hydrogenation

This work investigates the effects of Au³⁺/Au⁰ ratio or distribution of gold oxidation states in Au/ZrO₂ catalysts of different gold loadings (0.01–0.76% Au) on CO oxidation and 1,3-butadiene hydrogenation by regulating the temperature of catalyst calcination (393–673 K) and pre-reduction with hydrogen (473–523 K). The catalysts were prepared by deposition–precipitation and were characterized with elemental analysis, nitrogen adsorption/desorption, TEM, XPS and TPR. The catalytic data showed that the exposed metallic Au⁰ atoms at the surface of Au particles were not the only catalytic sites for the two reactions, isolated Au³⁺ ions at the surface of ZrO₂, such as those in the catalysts containing no more than 0.08% Au were more active by TOF. For 0.76% Au/ZrO₂ catalysts having coexisting Au³⁺ and Au⁰, the catalytic activity changed differently with varying the Au³⁺/Au⁰ ratio in the two reactions. The highest activity for the CO oxidation reaction was observed over the catalyst of Au³⁺/Au⁰ = 0.33. However, catalyst with a higher Au³⁺/Au⁰ ratio showed always a higher activity for the hydrogenation reaction; co-existance of Au⁰ with Au³⁺ ions lowered the catalyst activity. Moreover, the coexisting Au particles changed the product selectivity of 1,3-butadiene hydrogenation to favor the formation of more trans-2-butene and butane. It is thus suggested that for better control of the catalytic performance of Au catalyst the effect of Au³⁺/Au⁰ ratio on catalytic reactions should be investigated in combination with the particle size effect of Au.     

The preparation of Au/CeO2 catalysts and their activities for low-temperature CO oxidation

Au/CeO₂ catalysts prepared by co-precipitation (CP) and deposition-precipitation (DP) methods were tested for low temperature CO oxidation reaction. The structural characters and redox features of the catalysts were investigated by XRD, XPS and H₂-TPR. Their catalytic performances for low temperature CO oxidation were studied by means of a microreactor -GC system. It showed that the catalytic activities of Au/CeO₂ catalysts greatly depended on the preparation method. The catalysts prepared by DP method exhibited a surprisingly higher activity towards CO oxidation than that prepared by CP method. This may arise from the differences in the particle sizes of Au and redox properties of the catalysts. The low Au loading and the resistance to high temperature of DP-prepared catalyst made it more applicable.     

Synthesis and characterization of CuO/TiO2 catalysts for low-temperature CO oxidation

In this paper, the CuO/TiO₂ catalysts prepared by the deposition–precipitation (DP) method were extensively investigated for CO oxidation reaction. The structural characters of the CuO/TiO₂ catalysts were comparatively investigated by TG-DTA, XRD, and XPS measurements. It was shown that the catalytic behavior of CuO/TiO₂ catalysts greatly depended on the TiO₂-support calcination temperature, the CuO loading amount and the CuO/TiO₂ catalysts calcination temperature. CuO supported on the anatase phase of TiO₂-support calcined at 400 °C showed better catalytic activity than those supported on TiO₂ calcined at 500 and 700 °C. Among all our investigated catalysts with CuO loading from 2% to 12%, the catalyst with 8 wt% CuO loading exhibited the highest catalytic activity. The optimum calcination temperature of the CuO/TiO₂ catalysts was 300 °C. The XRD results indicated that the catalytic activity of the CuO/TiO₂ catalysts was related to the crystal phase and particle size of TiO₂ support and CuO active component.     

制备条件对Au/TiO_2液相氧化反应活性的影响

采用沉积-沉淀法制备纳米级Au/TiO_2催化剂,以葡萄糖液相催化氧化制葡萄糖酸为探针反应,考察了催化剂制备条件对Au/TiO_2活性的影响,并利用TEM、XRD和XPS等方法对催化剂进行了表征。结果表明,Au/TiO_2对葡萄糖液相氧化反应的催化活性与催化剂的制备条件密切相关,纳米金的颗粒尺寸不是决定催化活性的惟一因素,金在催化剂中的价态对催化活性有重要影响。     

钴基催化剂的制备及性能评价

以γ-Al_2O_3为载体,采用等体积浸渍法制备F-T合成钴基催化剂,在F-T合成小型固定床反应装置评价催化剂。考察并优化了钴源、焙烧温度、钴负载量、反应温度和原料气空速等工艺条件对催化荆活性和F-T合成产物收率的影响,测试了Co/γ-Al_2O_3催化剂的稳定性。结果表明,最佳制备条件:以硝酸钴为钴源,焙烧温度400℃,钴负载质量分数10%。在温度230℃、压力2 MPa、原料气组成n(H_2)∶n(CO)=2和反应空速1 800 h~(-1)的条件下,进行60 h运转实验,CO转化率可达69.1%,C_5~+烃收率高达89.6%。     

Complete oxidation of 2-propanol over gold-based catalysts supported on metal oxides

This paper concerns the preparation of metal oxide-supported gold catalysts and their application to 2-propanol abatement in order to lower the light off temperature. Catalytic oxidation of 2-propanol was investigated on Au/CeO₂, Au/Fe₂O₃, Au/TiO₂ and Au/Al₂O₃ catalysts prepared from the deposition–precipitation (DP) method. The catalysts are characterized by XRD (X-ray diffraction), BET (Brunner–Emmett–Teller), TEM (transmission electron microscopy), NH₃-TPD (NH₃-temperature programmed desorption), H₂-TPR (H₂-temperature programmed reduction), ICP-AES (inductively coupled plasma-atomic emission spectroscopy) and XPS (X-ray photoelectron spectroscopy) techniques. The catalytic activity of Au/metal oxide samples towards the deep oxidation of 2-propanol to CO₂ and water has been found to be strongly dependent on the kind of supports, the amount of gold loading, the calcination temperature and the moisture content in the feed.     

Enhancement of catalytic activity of Au/TiO2 by thermal and plasma treatment

A significant enhancement in the catalytic activity of Au/TiO₂ in CO oxidation and preferential oxidation reaction by creating the active sites on the catalyst surface by thermal treatment as well as by producing small gold particles by plasma treatment has been studied. Au/TiO₂ catalyst (Au (1 wt%) supported on TiO₂) was prepared by conventional deposition-precipitation method with NaOH (DP NaOH) followed by washing, drying and calcination in air at 400 °C for 4 h. Thermal treatment of Au/TiO₂ was carried out at 550 °C under 0.05 mTorr. A small amount of Au/TiO₂ catalyst was taken from the untreated and thermally treated Au/TiO₂ and both kinds of catalysts were treated with plasma sputtering at room temperature. The activity of the catalysts has been examined in the reaction of CO oxidation and preferential oxidation (PROX) at 25–250 °C. Thermally treated Au/TiO₂ showed better catalytic activity as compared to the untreated catalyst. There is also an additional enhancement in the catalytic activity due to plasma sputtering on the both kinds of catalysts. Thermally treated Au/TiO₂ followed by plasma sputtering Au/TiO₂ showed higher conversion rates for CO oxidation reaction compared with untreated, thermally treated and plasma sputtered Au/TiO₂ catalysts. It may be concluded that the enhancement of catalytic activity of thermally treated Au/TiO₂ followed by plasma sputtering is owing to the generation of active sites such as oxygen vacancies/defects in TiO₂ support using thermal treatment as well as by producing small gold particles using plasma treatment.