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考察了以拟薄水铝石为铝源、固体硅胶为硅源、四乙基氢氧化铵为模板剂时不同晶化混合液SiO2/Al2O3比和不同晶化温度对β沸石合成的影响。XRD、TGA、ICP及SEM研究结果表明,在晶化混合液SiO2/Al2O3比为20至50之间、晶化温度为140℃~160℃范围内能合成出高结晶度的β沸石,且β沸石硅铝比与晶化混合液硅铝比呈良好的线性关系:TGA总失重量随β沸石硅铝比增加而增加,晶化温度对β沸石的晶粒度没有明显影响。此外,所制备的Hβ沸石对甲苯与C9芳烃歧化和烷基转移反应具有良好的催化性能。 相似文献
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在V2O5/TiO2催化剂中分别添加Li、K、Cs等碱金属离子,利用BET、XRD、XPS、H2TPR、O2-TPD-MS和化学分析方法,研究了催化剂结构和性能的变化。结果表明,催化剂在添加不同碱金属离子 后,其结构表面活性氧发生了很大变化,K离子可以改善催化剂的活性、提高反应选择性;Li离子能提高催化剂活性,但在相当宽的温度范围内使反应选择性下降;在693K以下,Cs离子对催化剂的活性和选择性均 相似文献
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以1,3,5-TMB和1,2,4-TMB转化为模型反应,探讨了铝柱联合成皂石(简称Al-PSS)上表面酸性质的特点。结合不同脱附温度下吡啶吸附量及NH_3-TPD研究,实验证明,Al-PSS表面具有数目较多,强度较大的酸性中心 和较弱的碱性中心 ,与铝柱联天然膨润土(简称Al-CLB)比较,有较高的脱烷基选择性。两种三甲苯在Al-PSS上的转化,不论是单一反应物还是二者混合反应物,其产物分布基本相同,四甲苯在其异构体中含量均高达80%,说明在本研究反应条件下,两种探针分子以Al-PSS为催化剂进行转化,其产物结构由催化剂结构和性质决定。 相似文献
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甲苯气相选择氧化制苯甲醛 Ⅳ.助剂锂、钾、铯对V_2O_5/TiO_2催化剂性能的影响 总被引:1,自引:0,他引:1
在V2O5/TiO2催化剂中分别添加Li、K、Cs等碱金属离子,利用BET、XRD、XPS、H2-TPR、O2-TPD-MS和化学分析方法,研究了催化剂结构和性能的变化.结果表明,催化剂在添加不同碱金属离子后,其结构和表面活性氧发生了很大变化.K离子可以改善催化剂的活性、提高反应选择性;Li离子能提高催化剂活性,但在相当宽的温度范围内使反应选择性下降;在693K以下,Cs离子对催化剂的活性和选择性均起抑制作用. 相似文献
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EFFECT OF CATALYST CONCENTRATION ON CATALYTIC PERFORMANCE IN LIQUID PHASE DIMETHYL ETHER SYNTHESIS FROM SYNGAS 下载免费PDF全文
利用ZSM-5型沸石可将轻烃选择性地转化为苯,甲苯和二甲苯。HZSM-5催化剂上丙烷转化率和芳烃选择性都很低,但在HZSM-5上添加Ga或Pt-Ga(双金属改性)后丙烷转化率和芳烃选择性都有很大提高。实验结果表明,Ga/HZSM-5催化剂经氢气高温预处理后,其上的Bro..nsted酸中心数目减少。铂的加入促进了镓物种的还原,而还原的镓物种可以中和相当一部分催化剂表面Br.nsted酸中心,然后形成高度不饱和的催化活性中心。这些中心可以作为Lewis中心,从丙烷和反应中间产物中拔除H-,使丙烷高选择性地生成芳烃 相似文献
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应用XRD,XPS,Mossbauer谱,TPR,CO化学吸附CO-TPD,CO+H2反应性能测试等手段研究了锰助剂对F-T合成制低碳烯烃Mn-Fe/ZrO2催化剂结构及催化性能的影响。结果表明,与Fe/Zr催化相比,加锰助剂后的催化剂F-T反应催化活性上升,甲烷选择性降低,低碳烯烃选择性增加。 相似文献
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硅烷化处理的纳米ZSM-5的结构表征及催化性能 总被引:2,自引:0,他引:2
采用多次浸渍法和化学反应沉积法对纳米HZSM-5分子筛外表面进行了硅烷化处理,考察了改性后纳米ZSM-5对甲苯歧化的催化活性.采用改进的Hammett指示剂法和吡啶吸附红外光谱研究了催化剂的酸性位,采用X射线衍射和29Si MASNMR对催化剂的结构进行了表征.研究结果表明,硅烷化处理降低了纳米ZSM-5酸性位的浓度,从而降低了纳米ZSM-5的催化活性.硅烷化处理还减少了纳米ZSM-5中Si的Q4物种,降低了纳米ZSM-5的相对结晶度,同时硅烷化处理产生了脱铝作用.骨架铝含量的减少导致催化剂的酸性位减少,催化活性降低. 相似文献
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Studies on Oxide Catalysts. XLV. Conversion of Aromatics on Dealuminated Zeolites ZSM-5 The catalytic properties of zeolites ZSM-5 dealuminated by hydrochloric acid are investigated in the isomerization of m-Xylene, the disproportionation of toluene and in the alkylation of toluene with methanol. Besides the increase of the Si/Al ratio, the dealumination leads to an inversion of the Si/Al concentration gradient in crystallites, to a shift of acidity spectrum and consequently to a change in catalytic activity and selectivity. 相似文献
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The catalytic properties of MCM-22 and NU-87 were investigated for the disproportionation of toluene to produce benzene and
xylene, and the results were compared with those obtained over mordenite, beta and ZSM-5. It turns out that dealumination
of MCM-22 removes selectively the acid sites from the external surface and thus suppresses the secondary isomerization of
p-xylene, enhancing the para-selectivity. This indicates that the dealuminated MCM-22 is a promising catalyst for the selective formation of p-xylene from toluene disproportionation.
This revised version was published online in June 2006 with corrections to the Cover Date. 相似文献
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合成了一系列硅铝比为31—176的ZSM-11沸石,以甲苯-甲醇烷基化、间二甲苯异构化和甲苯歧化三个反应作为探针反应,研究了它们的催化性能。将其与酸性质和晶胞参数相关联发现,低硅铝比适于甲苯歧化,中硅铝比适于间二甲苯异构化,高硅铝比适于甲苯-甲醇烷基化反应。各反应所需的酸强度为甲苯歧化>间二甲苯歧化>间二甲苯异构化>甲苯-甲醇烷基化。Na~+的存在以及用4-甲基喹啉或(CH_3)_3SiCl中毒,可抑制强酸位,明显提高甲苯-甲醇烷基化反应生成对二甲苯的选择性,尤以(CH_3)_3SiCl中毒的低Al/u.c.的NaHZSM-11最佳。 相似文献
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以贵金属改性的钙钛矿为活性组分,通过等体积浸渍法制备了Pd/La0.8Ce0.2MnO3/ZSM-5催化剂,并采用XRD、BET、SEM和H2-TPR等技术对催化剂进行了表征。在固定床反应器上,对Pd/La0.8Ce0.2MnO3/ZSM-5催化剂上的甲苯为目标污染物的催化燃烧进行了研究,考察了焙烧温度、负载量及ZSM-5的性质对其催化活性的影响。结果表明,所得到Pd/La0.8Ce0.2MnO3催化剂仍保持钙钛矿型结构,Pd均匀的分布在催化剂表面,有利于催化剂活性的提高。当ZSM-5硅铝原子比为25、La0.8Ce0.2MnO3负载量为20%、焙烧温度为750℃时,La0.8Ce0.2MnO3/ZSM-5上甲苯的起燃温度和完全转化温度分别为200和279℃;加入0.3%的Pd后,Pd/La0.8Ce0.2MnO3/ZSM-5的催化活性明显提高,甲苯起燃温度下降了90℃,完全转化温度可低至230℃。 相似文献
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Vesselina Mavrodinova Margarita Popova Magdolna R. Mihályi Gabriella Pál-Borbély Christo Minchev 《Reaction Kinetics and Catalysis Letters》2004,83(2):345-352
The catalytic performance of MCM-22 modified with Cs to different extents by Solid-State Ion Exchange has been investigated
in toluene disproportionation. It was suggested that protons on the external surface were preferentially replaced by Cs cations.
It was observed that the Cs modifications did not provide improved p-xylene selectivity at conversions close to that of the H-form. The remaining unaffected proton sites in the 10 MR channels
are considered as responsible for secondary xylene isomerization proceeding upon toluene disproportionation.
This revised version was published online in June 2006 with corrections to the Cover Date. 相似文献
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Sankar M Nowicka E Tiruvalam R He Q Taylor SH Kiely CJ Bethell D Knight DW Hutchings GJ 《Chemistry (Weinheim an der Bergstrasse, Germany)》2011,17(23):6524-6532
In the solvent-free oxidation of benzyl alcohol to benzaldehyde using supported gold-palladium nanoparticles as catalysts, two pathways have been identified as the sources of the principal product, benzaldehyde. One is the direct catalytic oxidation of benzyl alcohol to benzaldehyde by O(2), whereas the second is the disproportionation of two molecules of benzyl alcohol to give equal amounts of benzaldehyde and toluene. Herein we report that by changing the metal oxide used to support the metal-nanoparticles catalyst from titania or niobium oxide to magnesium oxide or zinc oxide, it is possible to switch off the disproportionation reaction and thereby completely stop the toluene formation. It has been observed that the presence of O(2) increases the turnover number of this disproportionation reaction as compared to reactions in a helium atmosphere, implying that there are two catalytic pathways leading to toluene. 相似文献
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Toluene Alkylation to Selective Formation of p-Xylene over Co-Crystalline ZSM-12/ZSM-5 Catalyst 下载免费PDF全文
The alkylation of toluene with methanol to selective formation of p-xylene has been systematically studied. ZSM-12 (MTW)/ZSM-5 co-crystalline zeolite in 40:60 proportions have been synthesized by the same molar gel composition, but at different temperatures and periods than that of ZSM-12 and ZSM-5, separately. All the prepared samples are characterized by XRD, SEM, BET, and XRF. The activity of toluene alkylation was investigated with a mixture of toluene and methanol as a feed over the ZSM-12, ZSM-12/ZSM-5 co-crystalline, ZSM-5, and physical mixture of ZSM-12/ZSM-5. Prom characterization, it is observed that the ZSM-12/ZSM-5 co-crystalline material is different from that of ZSM-12, ZSM-5, and their physical mixture. Further, the ZSM-12/ZSM-5 co-crystalline zeolite produces the highest content of xylene and has better selectivity for p-xylene than ZSM-12, ZSM-5, and their physical mixture. 相似文献