共查询到20条相似文献,搜索用时 171 毫秒
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采用表面改性法制备了负载型Ni2(OCH3)2/SiO2双核金属甲氧基配合物催化剂,利用IR、DSC、TPD和微反技术对催化剂的表面结构、化学吸附性质和催化活性进行了研究。结果表明,负载型双核金属甲氧基配合物Ni2(OCH3)2/SiO2中Ni^2 与载体SiO2表面O^2-以双齿配位形式键合;二氧化碳在催化剂表面存在桥式吸附态和甲氧碳酸酯基物种两种吸附态,丙烯则只有一种吸附态;在适宜反应条件下,CO2和丙烯在Ni2(OCH3)2/SiO2催化剂上可以高选择性地合成甲基丙烯酸,反应物分子共吸附于催化剂表面同一活性单元以及羧酸根与丙烯解离吸附态的形成是反应顺利进行关键因素. 相似文献
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加氢催化剂预硫化技术探讨 总被引:11,自引:1,他引:10
1前言加氢催化剂大多采用Mo、Co、Ni、W等金属元素作组分,并以氧化态分散在多孔的载体上。大量的研究试验结果表明,这种形态的催化剂加氢活性低,活性稳定性差。若将催化剂经过预硫化处理,即在硫化剂和氢气存在下使氧化态金属转化为硫化态金属,则硫化态催化剂的活性和稳定性均高于氧化态催化剂。催化剂预硫化技术是加氢催化剂开发应用的关键步骤之一。当今,随着催化剂制备技术的发展,促进了国内外对加氢催化剂预硫化技术的基础研究和应用研究。最佳的预硫化技术能够使加氢催化剂保持最佳的加氢活性和活性稳定性,提高催化剂的选择性… 相似文献
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氯氟烃加氢脱氯催化剂的研究进展 总被引:3,自引:0,他引:3
从氯氟烃(CFCs)选择性加氢脱氯催化剂的催化活性组分、活性组分前驱体、载体及裁体-金属相互作用、双金属催化剂、催化剂的结构敏感性和催化剂失活等方面详细介绍了CFCs选择性加氢脱氯反应及催化剂的最新研究进展,并指出了CFCs选择性加氢脱氯反应的发展方向。 相似文献
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负载型铬基催化材料不仅可显著提高铬活性组分的分散度并保留其多价态性,同时兼具多孔载体材料固有的孔结构、强酸性及优异的分子扩散性能,从而表现出良好的催化活性,并作为一类重要的催化剂有效应用于多种催化过程。本文详细阐述了目前负载型铬基催化剂在制备方法及催化应用方面的研究进展,并就合成方法、载体性质、金属前体及助剂等因素对铬物种引入量、分散程度及配位状态的影响以及进而造成对催化剂孔道结构、反应活性及使用寿命的影响进行了详尽地评述。同时指出了通过改变载体的表面酸性、孔结构及其与活性组分铬物种间的相互作用,从而提高铬物种在载体中的分散度和稳定性是今后负载型铬基催化材料研究的重要方向。 相似文献
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用SiO2担载壳聚糖(CS),再与PdCl2配位,制得催化剂SiO2-CS-PdCl2,详细考察了催化剂对有机锡试剂和α-卤代酸酯交叉偶联反应的催化作用及使用寿命。结果表明该天然高分子负载型钯催化剂对偶联反应具有较高的催化活性和化学选择性,分离容易,可以重复使用,酯基在反应中不被破坏。催化剂循环使用6次,偶联反应产率仍在40%以上。采用XPS分析方法对催化剂进行了表征,证明催化活性中心是金属态钯,并对反应机理进行了研究和探讨。 相似文献
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Pt与载体间的相互作用会影响到本征Pt纳米粒子的催化活性,不同Pt前体制备Pt/CeO2催化剂会使其表现出完全不同的催化性能。分别采用金属胶体粒子原位沉积法、浸渍法以及浸渍还原的方式制备了Pt/CeO2催化剂,通过X 射线衍射、程序升温还原、X射线光电子能谱以及高分辨透射电镜对催化剂进行表征,在CO氧化以及甲苯燃烧反应中评价催化剂活性。结果表明,胶体粒子原位沉积法制备Pt/CeO2催化剂,能够将优先合成好的Pt纳米粒子直接以金属态Pt0的形式负载到载体表面,且保证其高度均匀分散,丰富的表面Pt0很好地充当了CO、甲苯反应时的活化位点,催化剂表现出优异的性能;浸渍还原法中,Pt纳米粒子之间会发生团聚现象,同时部分Pt又以Pt2+的形式与CeO2之间形成了Pt-O-Ce相互作用,载体表面暴露Pt0含量的下降是催化剂表现出较弱活性的主要原因;浸渍法中,以Pt离子对Pt进行负载,Pt完全以Pt2+的形式参与到Pt-O-Ce键成键中,表面Pt0缺失,催化剂表现出明显的失活现象。Pt/CeO2催化剂中,起主要活性作用的是金属态Pt0,胶体粒子原位沉积法能够实现Pt0的直接负载,对于提高Pt基催化剂中Pt的利用率,降低Pt资源消耗都具有重要意义。 相似文献
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Hydroprocessing catalysts based on Ni, Co, Mo and W are used in various refinery processing applications where several deactivation mechanisms become of importance (coke formation, active phase sintering, metals deposition, poisoning) in the catalyst's life cycle. The life cycle of commercial hydroprocessing catalysts is very complex and includes the catalyst production, sulfidation, use, oxidative regeneration followed by re-sulfidation and reuse or, if reuse is not possible, recycling or disposal. To understand the changes in catalyst properties taking place during a life cycle, the catalyst quality in the different stages can be best monitored by using advanced analytical techniques. The catalyst's life cycle is further complicated by numerous technical, environmental and organizational issues involved. In principle, different companies can be involved in each of the life cycle steps. Leading catalyst manufacturers, together with specialized firms, offer refineries a total catalyst management concept, starting with the purchase of the fresh catalyst and ending with its final recycling or disposal. Total catalyst management includes a broad range of services, ensuring optimal timing during the change-out process, reliable, smooth and safe operations, minimal downtime and maximum catalyst and unit performance. 相似文献
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探讨了常压气相法甲醇氧化羰基化合成碳酸二甲酯(DMC)的小试,在10ml催化剂、900~2000h-1空速条件下,用连续流动固定床反应体系,研究了氮气的稀释量对催化活性的影响,42%的氮气含量为最佳;同时研究了不同的活性炭载体及不同的金属添加成分对负载型钯催化剂的催化活性与DMC选择性的显著影响,其中用Pd Cu/煤质炭催化剂得率为101mmol/g·h,相应地DMC选择性达95%。还探讨了催化剂的预处理对反应活性的影响,为进一步的放大试验提供了重要信息 相似文献
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对加压法二氧化碳与环氧丙烷合成碳酸丙烯酯催化剂进行了研究,实验结果表明:KI/聚乙二醇400催化体系具有很好的催化活性,可在较低温度、压力下短时间高产率的得到碳酸丙烯酯。碳酸丙烯酯得率可达99.8%以上,在一定条件下。经多次循环使用后仍有较高的活性。 相似文献
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P. S. Voskanyan 《Catalysis in Industry》2010,2(2):167-172
The activity, selectivity, and service life of a palladium-, gold-, and potassium acetate-containing catalyst for vinyl acetate
(VA) synthesis are reported as a function of the catalyst composition. Equations relating these performance parameters to
the percentage of each component are suggested. General relation-ships between the catalytic activity and the component contents
are established for optimization of the catalyst composition. These relationships have been validated by bench tests. The
average activity of the 1.5% Pd + 0.75% Au + 5.0% KOAc catalyst is 700 (g VA)/(l Cat h), and its ethylene-to-VA conversion
selectivity is 93–95%. 相似文献
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New evidence for the structure of Ni-catalyzed stacked-cup carbon nanofibers (CNFs) has been found. This type of carbon nanofiber exhibits a wide hollow core as well as a large diameter (between 40 and 140 nm). The fibers have been produced by the floating catalyst method using natural gas as carbon feedstock, a sulfur compound, and a nickel catalyst. It was found that the catalytic particles are heterogeneous with two different parts: one composed of metallic Ni, which is the catalytically active portion of the particle, and another composed of NiS, which allows for the hollow nanofiber structure. The hollow core of the fibers has similar dimensions to the NiS volume of the particle and the graphitic layers grow from the rear nickel region of the particle. Nevertheless, the NiS component seems to be indispensable in producing the helix-spiral formation of the graphitic structure, as clearly shown by the TEM studies. 相似文献
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Santhosh Kumar Matam Gian Luca Chiarello Ye Lu Anke Weidenkaff Davide Ferri 《Topics in Catalysis》2013,56(1-8):239-242
The oxidation state of palladium in a model Pd/ACZ three-way catalyst was monitored by synchronous XANES and mass spectrometry during two consecutive heating (to 850 °C) and cooling (to 100 °C) cycles under stoichiometric conditions simulating exhaust after treatment of a natural gas engine. During heating in the first cycle, PdO reduction occurred around 500 °C and the initial fully oxidized state of Pd was never recovered upon heating and cooling cycles. A mixed Pd2+/Pd oxidation state was at work in the second cycle. Hence, the operando XANES study reveals that the PdO x /Pd pair exists in a working catalyst but is less active than the catalyst in its initial state of fully oxidized palladium. It is also evident from XANES spectra that ceria–zirconia promotes re-oxidation of metallic Pd, thus reasonably sustaining catalytic activity after exposure to high temperatures. 相似文献
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Well‐dispersed PtSnEu/C and PtSn/C catalysts were prepared by the impregnation–reduction method using formic acid as a reductant and characterised by X‐ray diffraction (XRD), transmission electron microscopy (TEM), energy dispersion X‐ray spectroscopy (EDX) and X‐ray photoelectron spectroscopy (XPS). The synthesised catalysts with different atomic ratios of Pt/Sn/Eu have the Pt face centered cubic (fcc) structure and their particle sizes are 3–4 nm. The PtSnEu/C catalyst is composed of many Pt (0), SnO2, Eu(OH)3, a small amount of Pt(II) and partly alloyed PtSn, but no metallic Eu. The electrochemical measurements indicate that in comparison with Pt3Sn1/C catalyst, the Pt3Sn1Eu1/C catalyst for ethanol oxidation has more negative onset potential, smaller apparent activation energy and lower electrochemical impedance so that it exhibits very high catalytic activity. Its peak current density increases by 135% and 40%, compared with Pt3Sn1/C and Pt1Ru1/C (JM) catalysts, respectively. This is because the Eu(OH)3 formed by adding Eu to PtSn/C catalyst can provide the OH group which is in favour of the removal of adsorbed intermediates and ethanol oxidation. 相似文献