首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 15 毫秒
1.
用沉积沉淀法制备了Au-CuO/TiO2催化剂和Au/TiO2催化剂,考察了沉淀温度、沉淀pH、焙烧温度和Cu/Au摩尔比等制备工艺条件对Au-CuO/TiO2催化剂性能的影响,确定了适宜的催化剂制备工艺条件.结果表明,Au-CuO/TiO2催化剂对CO2中微量H2的脱除具有较好的活性和稳定性.还考察了还原和H2S中毒处理先后的顺序对催化剂H2脱除活性的影响.结果表明,Au/TiO2催化剂基本上不受处理顺序的影响,而H2S处理顺序对Au-CuO/TiO2催化剂的性能有较为明显的影响,这说明还原后的Au-CuO/TiO2催化剂形成了Au-Cu合金。  相似文献   

2.
郭强  吴美玲  刘源  白雪 《催化学报》2007,28(11):953-957
采用溶胶-凝胶法制备出介孔氧化铈(meso-CeO2)及其负载的氧化钴(Co3O4/meso-CeO2)催化剂,并将其应用于富氢气体中CO的优先氧化反应.通过N2物理吸附及X射线衍射表征考察了meso-CeO2和Co3O4/meso-CeO2的结构性质.活性评价结果表明,在高空速下,Co3O4/meso-CeO2催化剂上的CO优先氧化性能很好,但水和CO2对CO的氧化有一定的负作用.Co3O4/meso-CeO2催化剂的CO完全氧化温度窗口远大于沉淀法制备CeO2负载的氧化钴催化剂.  相似文献   

3.
富氢条件下Au/γ-Al2O3催化剂上CO的选择氧化反应   总被引:3,自引:0,他引:3  
 用脉冲反应考察了富氢条件下Au/γ-Al2O3催化剂上CO的选择氧化反应.结果表明,CO和O2在Au/γ-Al2O3催化剂表面同时发生吸附,其吸附活性中心都在催化剂的活性组分表面,CO的吸附强度大于O2的吸附强度,吸附态的CO和吸附态的O2之间反应生成CO2.提高反应温度和增加原料中氧的含量都能提高CO的转化率.在所考察的实验条件下,O2的反应选择性基本上为100%.  相似文献   

4.
张启俭  齐平  周迎春 《催化学报》2008,29(4):361-365
以Fe2O3,Co3O4,ZrO2和ZrO2-CeO2为载体,研究了负载型Au催化剂在CO优选氧化反应中的性能,并用高分辨透射电子显微镜、X射线衍射和X射线光电子能谱等技术对催化剂进行了表征,考察了Au与载体之间的相互作用对Au电子性质的影响.结果表明,在60℃以下,Au/Fe2O3上CO能被完全氧化,且CO氧化反应选择性约为50%,而在Au/Co3O4,Au/ZrO2和Au/ZrO2-CeO2催化剂上,CO在更低的温度下才能被完全氧化.这是由于具有拉电子效应的载体(如Fe2O3和Co3O4)能使Au带有部分正电荷,从而对CO优选氧化反应具有较高的催化活性.因此,选择合适的载体或对载体进行掺杂改性,调节Au的正电荷数目,有可能进一步提高Au催化剂的催化活性.  相似文献   

5.
采用多元醇为模板剂合成了介孔Ce1-xZrxO2(x=0.2,0.35,0.5)固溶体材料,并以其为载体负载CuO制备了Cu基催化剂.应用透射电子显微镜、X射线衍射、程序升温还原、程序升温脱附和N2吸附-脱附等技术对载体及催化剂进行了表征,并研究了Zr的取代比例x值对载体和Cu基催化剂性能的影响.结果表明,所有Ce1-xZrxO2样品均为介孔材料,其中Ce0.5-Zr0.5O2载体样品有较大的比表面积(181m2/g),CuO/Ce0.5Zr0.5O2催化剂样品在富氢条件下有较高的催化CO选择性氧化反应的活性和选择性.与其他催化剂样品相比,CuO/Ce0.5Zr0.5O2催化剂样品中形成的活性中心更多,分散性更好,对CO的吸附量更大,CO脱附温度更低,活性组分与载体的相互作用更强。  相似文献   

6.
超临界流体中CO和H2吸附过程的Monte Carlo模拟   总被引:2,自引:0,他引:2  
利用Monte Carlo (MC) 方法,研究了一氧化碳和氢气在不同密度正己烷中的等温吸附情况.模型考虑了正己烷密度对一氧化碳和氢气在催化剂表面吸附量与吸附速率的影响.结果表明,主要有三个因素会影响溶质的吸附量:当溶剂密度低于其临界密度时,体系压力是影响溶质吸附量的主要因素;当体系处于超临界区时,超临界溶剂的溶解能力以及溶质和溶剂之间的竞争吸附是影响溶质吸附量的主要因素.在一定范围内增加溶剂的密度(压力)可以提高溶质在催化剂表面的吸附速率.  相似文献   

7.
 采用程序升温与原位FT-IR,CO程序升温脱附和X射线衍射等技术研究了钾对Rh/Al2O3催化剂上CO吸附态和表面吸附物种的影响. 结果表明,钾未改变金属铑上CO吸附的形态,但削弱了CO的吸附强度; 在程序升温(真空中)的动态过程中,120 ℃时CO线式吸附完全脱除,180 ℃时CO桥式吸附完全脱除; 助剂钾明显促进了表面甲酸盐和碳酸盐物种的形成,同时减弱了Al-Rh的相互作用. 讨论了钾存在时甲酸盐和碳酸盐物种的形成机理.  相似文献   

8.
CH4+CO2H2+CO     
将廉价的碳源(CO2)转化为化石燃料可缓解由于温室气体引起的气候问题.CH4/CO2重整(CRM)是CO2转化利用的有效途径之一,要实现这个过程的关键是研制高效的光响应催化剂.本文采用WO3负载的第VIII族金属催化剂、引入光照能量来活化CO2,利用光热协同催化CRM.研究结果表明,光学材料WO3负载的第VIII族金属催化剂在可见光辅助下的催化活性是热驱动条件下的1.4~2.4倍,与等离子体金催化剂的活性增强率(1.7倍)相当.进一步以不同波段的可见光为光源,对WO3负载的第VIII族金属催化剂上催化活性提高的原因进行了研究.结果表明,活性增强率与WO3在可见光区域的吸光趋势并不吻合,说明并非WO3提高了其负载的第VIII族金属催化剂上CRM活性.除WO3外, WO3-x亦可作为光催化剂吸收可见光,因此,本文通过X射线光电子能谱、X射线衍射及紫外-可见分光光度法等进行表征.结果表明,在还原型CRM反应气氛下, WO3部分原位还原为WO3-x,并且活性增强率与WO3-x在可见光区域的吸光趋势相吻合,说明导致可见光辅助下活性增强的是WO3-x而不是WO3.热力学分析及原位电子顺磁共振波谱法结果表明, CO2的活化是CRM的速控步,该步骤吸热,在500 oC时不能自发进行.在可见光的辅助下, CO2可以被WO3-x通过Mars-vanKrevelen机理进行活化,提高速控步的反应速率,进而提高了催化活性.综上,本文为提高光催化活性提供了一条有效途径.  相似文献   

9.
研究了MOx(M=Co,Mn,Al和La)对CuO/CeO2催化剂富氢条件下CO选择性氧化性能的影响,并运用XRD,XPS,BET,TPR和TPD等手段对催化剂进行了表征.结果表明,MnOx和Co3O4的引入能提高CuO/CeO2催化剂富氢条件下CO选择性氧化的活性,其中以MnOx的改性效果最好,80 ℃时CO转化率达58%,140℃为100%.与其他CuO/CeO2-MOx催化剂相比,CuO/CeO2-MnOx催化剂中活性组分与载体的相互作用较强,铜原子外电子云密度升高,表面Cu和晶格氧含量较多,CO的吸附量较大.  相似文献   

10.
The stability and curvature of emulsions of H2O and CO2 are reported and analyzed in terms of measurements of interfacial tension versus formulation variables, including salinity, CO2 density, temperature and pH. Among the surfactants studied are, quaternary ammonium cationic ones with perfluoropolyether tails, block copolymer ionomers and a poly (hydroxyethyl methacrylate) with polydimethylsiloxane tails, and a nonionic ethylene oxide surfactant with a fluoroalkane tail. The interfacial tension measurements were made at surfactant concentrations from 0.05 to 1.0 wt% with a variable-volume pendant drop tensiometer up to 345 bar and 363°K. As a formulation variable was varied, the system reached a balanced state characterized by a minimum in interfacial tension, a loss in emulsion stability and in some cases an inversion from a W/C to C/W emulsion. Here the Marangoni-Gibbs stabilization weakens, and also it becomes easy to bend and rupture the surfactant monolayer, causing coalescence. Except in the case of the nonionic fluorinated surfactant C8F17—SO2NEt-(CH2CH2O)12–14CH3, the crossover from the CO2-continuous (W/C) to the H2O-continuous (C/W) emulsion occurred abruptly due to clouding of the surfactant out of the CO2 phase. For PFPE-TMAA, the plot of γ versus surfactant concentration revealed both pre-micellar aggregates and a critical micro emulsion, each of which was dependent on salinity.  相似文献   

11.
12.
用insituFTIR法研究了H2、CO及CO/H2在ZrO2表面的吸附行为.结果表明,H2在ZrO2表面吸附存在两种形态的羟基(即ZrOH和ZrOHZr),吸附温度增加,羟基数量增加.CO在200℃易与ZrO2表面羟基作用形成甲酸盐物种,吸附温度升高时,该物种逐渐分解生成CO和ZrOH.当CO和H2共存时,表面甲酸盐的量明显增加,并随温度增加,逐渐加氢形成甲氧基,最后生成甲烷.甲氧基的加氢过程较慢,所需反应温度也较高,被认为是CO加氢合成醇的速控步骤.  相似文献   

13.
14.
The contribution of N.T. Kudryavtsev (and later his son V.N. Kudryavtsev) to the development of electrodeposition science and technology, and especially to that of chromium, is inestimable. It is a privilege on this occasion to present some considerations of the two-phase nature of chromium electroplating solutions, caused by the generation of hydrogen gas and the use of vigorous air agitation, and to discuss its influence on fluid conductivity and consequent power consumption during electrodeposition.  相似文献   

15.
Swamps and tidal flats are believed to he important natural sources of atmospheric H2S, though it is very difficult to detect the low concentrations of this trace gas above the surface of these regions. In view of this problem an air sampling device has been developed for the sampling of atmospheric H2S with chemically impregnated filters. The sulfide generated on the filter is analyzed in a washing solution employing a very sensitive fluorescence method. The quality of the method is demonstrated by comparative calibrations. The fluorescence method is calibrated in the liquid phase with standard solutions of sulfide. Furthermore the sampling and analyzing method is calibrated together by using H2S calibration gases. The detection limit of the method is shown to he 10ng/m3 STP. Data of test-measurements in ambient air and some results of field-measurements in the lower troposphere are presented.  相似文献   

16.
17.
The effects of collision energy (Ecol) and five different modes of H2CO+ vibration on the title reaction have been studied over the center-of-mass Ecol range from 0.1 to 3.2 eV, including measurements of product ion recoil velocity distributions. Electronic structure and Rice-Ramsperger-Kassel-Marcus calculations were used to examine properties of various complexes and transition states that might be important along the reaction coordinate. Two product channels are observed, corresponding to Hydrogen Transfer (HT) and Proton Transfer (PT). Both channels are endothermic with similar onset energies of approximately 0.9 eV; however, HT dominates over the entire Ecol range and accounts for 70-85% of the total reaction cross section. Both HT and PT occur by direct mechanisms over the entire Ecol range, and have similar dependence on reactant vibrational and collision energy. Despite these similarities, and the fact that the two channels are nearly isoenergetic and differ only in which product moiety carries the charge, their dynamics appear quite different. PT occurs primarily in large impact parameter stripping collisions, where most of the available energy is partitioned to product recoil. HT, in contrast, results in internally hot products with little recoil energy and a more forward-backward symmetric product velocity distribution. Vibration is found to affect the reaction differently in different collision energy regimes. The appearance thresholds are found to depend only on total energy, i.e., all modes of vibration are equivalent to Ecol. With increasing Ecol, vibrational energy becomes increasingly effective, relative to Ecol, at driving reaction. For HT, this transition occurs just above threshold, while for PT it begins at roughly twice the threshold energy.  相似文献   

18.
庄林  周琴  陆君涛 《电化学》2000,6(1):10-16
本论文工作通过设计新型的电解池 ,首次实现了导电聚合物的电化学现场ESR_电导同步测量 .从获得的聚苯胺ESR信号及膜电阻随电极电势变化的精细图象看出 ,极化子晶格的形成与消亡决定了聚苯胺的导电行为 .从不同电势下聚苯胺的ESR饱和行为也得到Curie自旋与Pauli自旋相互转化的新证据 .  相似文献   

19.
Conductivity of cadmium acetate over the concentration range of 10?4 to 10?3M was measured at 25°C. The approximate dissociation constant of CdAc2 in dilute aqueous solution was estimated from the relation, α=[Λ?36.5+39√C(1+2α)]/[57.9?93√C(1+2α)]. The limiting value of log10K for the association constant of CdAc+ ion was evaluated to be 1.75 at 25°C.  相似文献   

20.
On the surface : Adsorption of O2 at the surface oxygen vacancy (SOV) sites of TiO2 reconstructs the lattice oxygen (healing SOVs), resulting in a decrease of the photocatalytic activity of oxidizing CO over vacuum‐pretreated TiO2 with increasing temperature (see scheme). Adsorption of H2 produces new SOVs at the TiO2 surface and stabilizes the photocatalytic activity.

  相似文献   


设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号