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1.
Fe/ZrO2气凝胶超细粒子催化剂的制备,表征及F—T反应性能的研究 总被引:4,自引:1,他引:4
用超临界流体干燥法制备出大孔高比表面高发散态Fe/ZrO2气凝胶超细粒子催化剂,研究了在其制备过程中织构性质、颗粒大小、体相和表面结构的变化,并与普通浸渍法制备的Fe/ZrO2催化剂作了对比。对几种Fe/ZrO2催化剂的F-T反应性能考察表明,Fe/ZeO2气凝胶超细催化剂显示出高的反应活性;随载体ZrO2颗粒尺寸减小,活性组分铁的分散度变大,其颗粒尺寸变小,催化剂比表面积增大,反应活性增大,甲烷 相似文献
2.
M(Fe,CO,Ni)ZrO2气凝胶超细粒子催化剂织构和结构热稳定性的研究 总被引:4,自引:0,他引:4
用超临界流体干燥(SCFD)法制备出高比表面纳米级ZrO2和M(Fe,Co,Ni)/ZrO2气凝胶超细原粉.详细考察了其在空气中450℃焙烧后织构和结构的变化,表明ZrO2气凝胶原粉织构和结构的热稳定性较差,而添加铁、钴、镍的M/ZrO2气凝胶原粉织构和结构的热稳定性明显增强,稳定作用依钴、镍、铁次序增加.焙烧后所得的M/ZrO2气凝胶超细催化剂颗粒增长不大,颗粒间仍较大程度地保持着原有凝胶三维网络织构状态.与常规法制备的催化剂相比,其比表面积和孔体积高出甚多. 相似文献
3.
采用共沉淀法与浸渍法制备了一系列SO42-/Fe2O3-ZrO2-SiO2固体酸催化剂,并将其用于催化乙酸/丁醉酯化反应。考察了以下影响催化剂活性的因素:Fe/Zr比、Si含量、制备方法、预焙烧温度和焙烧温度等。催化剂采用如下条件制备: Si含量为2 %, Fe/Zr比为 0.25,共沉淀法, 773 K焙烧,此时酯收率及生成酯的选择性可分别达到93.26%和96.01%。 SO42可能是活性组分之一。 相似文献
4.
调变钴系超细粒子催化剂合成重质烃 总被引:2,自引:0,他引:2
制备了SiO2气凝胶超细粉、ZrO-SiO2超细复合氧化物载体以及Co/ZrO2-SiO超细粒子催化剂,考察了还原温度对Co/ZrO2-SiO催化剂F-T反应性能的影响。结果表明,400下,H2还原的Co/ZrO2-SiO2催化剂有最佳F-T反应活性和C5选择性。 相似文献
5.
用XRD、TPR及固定床微反应器技术研究了微量Pt 和Pd 对Fe2O3/ZrO2 催化剂结构及性能的影响。结果表明,活性组分Fe3 + 与载体ZrO2 之间的相互作用会阻止载体从无定形ZrO2 到t-ZrO2 进而m - ZrO2 的转变,同时,促进Fe2O3 在ZrO2 表面的分散。微量Pt 或Pd 的加入对Fe2O3 在ZrO2 上的分散状态无明显影响,但使Fe2O3/ZrO2 的还原性能发生明显变化,表层Fe2O3 的还原性显著增强,导致M- Fe2O3/ZrO2 催化剂在NO+ CO反应中有更高的催化活性。N2 生成的选择性次序为Fe2O3/ZrO2 > Pd - Fe2O3/ZrO2 > Pt- Fe2O3/ZrO2 > Pd/ZrO2 > Pt/ZrO2 。 相似文献
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7.
Co基超细粒子催化剂用于合成重质烃Ru助剂的作用 总被引:3,自引:0,他引:3
用溶胶凝胶法制备了SiO2气凝胶超细粉体及ZrO2SiO2超细复合载体,用浸渍法制备了Co/ZrO2SiO2超细粒子催化剂并用干混法制备了CoRu/ZrO2SiO2催化剂.考察了Ru的添加对Co/ZrO2SiO2催化剂的织构、结构、还原、氢脱附及其FT反应性能的影响.结果表明,Ru的添加使Co2+更难还原,催化剂活性略有下降,CH4选择性降低,C5+选择性及收率升高;Co1%Ru/ZrO2SiO2催化剂上的烃类产物不遵从SchulzFlory分布,在C9和C15有两个最高峰. 相似文献
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9.
Fe_2O_3/ZrO_2催化剂上一氧化碳加氢反应制低碳烯烃──I.催化剂反应性能及反应过程中铁物相的变化 总被引:1,自引:0,他引:1
用浸渍法制得一系列不同铁负载量的Fe2O3/ZrO2催化剂,应用催化反应评价结合穆斯堡尔谱对催化剂的CO加氢反应性能、催化剂活性相结构及催化剂铁物种在合成气反应过程中的物相变化进行了研究.结果表明,铁负载量的大小对于Fe2O3/ZrO2催化剂的F-T反应催化性能有很大影响,铁负载量适当时,Fe2O3/ZrO2催化剂铁锆间适当的强相互作用使得催化剂在保持较高催化活性的同时高选择性地生成低碳烯烃,产物分布偏离Schulz-Flory分布规律. 相似文献
10.
作为甲醇氧化制甲醛、甲醇氨氧化制HCN反应的催化剂,其活性组分钼的流失是导致催化剂失活的主要原因。本文结合程序升温脱附(TPD)及X-光衍射(XRD)等测试手段,对Mo-Fe/SiO_2催化剂及工业实际用多元复合钼催化剂中钼的流失动力学和机理进行了研究。在HCN合成过程中,水能引起活性组分钼的流失,而水又是反应产物。对工业用多元复合钼催化剂的流失情况进行了动力学考察,实验发现,催化剂中的钼是较难流失的,XRD测试结果表明,Mo-Fe/SiO_2催化剂中的钼是以Fe_2(MoO_4)_3晶体形式存在的,而反应后催化剂中Mo为MoO_3晶体状态。与其它催化剂比较,MoO_3/SiO_2催化剂中的钼难流失,而较Bi-Mo/SiO_2催化剂中的钼易流失。其中工业用催化剂是最为稳定的。根据实验结果,结合我们以前的工作,证明Mo-Fe/SiO_2催化剂中,由于钼组分和铁组分的相互作用,使得Mo-Fe/SiO_2中的Mo的流失难于单组分的MoO_3/SiO_2催化剂,此外钼流失过程中MoO_2(OH)_2与催化剂中铁组分反应生成钼酸盐的倾向也是Mo难于流失的原因之一。而Mo-Fe/SiO_2和Mo-Bi/SiO_2催化剂中钼流失速度的差异 相似文献
11.
Uroš Grošelj Mojca Žorž Amalija Golobič Branko Stanovnik Jurij Svete 《Tetrahedron》2013,69(52):11092-11108
A new and simple synthesis of novel N-protected methyl 5-substituted-4-hydroxypyrrole-3-carboxylates, which exist in equilibrium with their 4-oxo tautomers, has been developed in two steps starting from N-protected α-amino acids. The key intermediates are enaminones, which can also be isolated, characterized, and used for the construction of other functionalized heterocycles, before they spontaneously decompose to pyrrole products. 4-Hydroxypyrroles are prone to partial aerial oxidation but can be efficiently alkylated or reduced to stable polysubstituted pyrrolidine derivatives. 相似文献
12.
The chemoselectivity in the intramolecular CH insertion of various diazosulfonamides has been experimentally studied. The results reveal that the aliphatic 1,4-, 1,5-, or 1,6-C(sp3)?H insertions of diazosulfonamides are not accessible, while the aromatic 1,5-C(sp2)?H insertion can be realized specifically by adjusting the diazo-adjacent group. In addition, the general chemoselectivities in the intramolecular CH insertions of diazosulfonyl compounds are summarized. Generally, diazosulfones undergo both aromatic 1,5-C(sp2)?H and aliphatic 1,5- and 1,6-C(sp3)?H insertions, while diazosulfonates undergo aliphatic 1,5- and 1,6-C(sp3)?H insertions. However, diazosulfonamides only undergo aromatic 1,5-C(sp2)?H insertion. 相似文献
13.
N-Heterocyclic carbene-palladacyclic complexes 3 were successfully achieved in a one-pot procedure under mild conditions. The structure of 3a was unambiguously confirmed by X-ray single crystal diffraction and it was an active catalyst in the Buchwald-Hartwig amination and α-arylation of ketones even at very low catalyst loadings (0.01?mol%). 相似文献
14.
Shashikant U. Dighe Surya K. Samanta Shivalinga Kolle Sanjay Batra 《Tetrahedron》2017,73(17):2455-2467
An efficient iodine-mediated oxidative Pictet-Spengler reaction in dimethyl sulphoxide (DMSO) using terminal alkynes as the 2-oxoaldehyde surrogate for the synthesis of aryl (9H-pyrido[3,4-b]indol-1-yl)methanones is described. The scope of the protocol includes the total synthesis of Fascaplysin, Eudistomins Y1 and Y2. The methodology is extended for preparing pyrrolo[1,2-a]-quinoxaline and indolo[1,5-a]quinoxaline derivatives. The utility of 1-aroyl-β-carbolines was demonstrated by performing palladium-catalyzed β-carboline directed ortho-C(sp2)-H functionalization of the phenyl ring with thiomethyl (SMe) group using DMSO as source and for accessing 4-aryl-canthin-6-ones. 相似文献
15.
In this Letter, we described a facile method for constructing fused bicyclic 1-arylpyrazol-5-one ring system. We employed various methylene-containing carboxylic acids as the substrates and proved that the pyrazolone ring closure requires activated methylene group in intermediate II. Accordingly, a series of structurally diversified, fused bicyclic 1-arylpyrazol-5-ones was prepared in moderate to high yields using the requisite substrates. 相似文献
16.
An efficient approach to the synthesis of highly congested di, penta and hexacyclic pyrazoles as well as imidazole fragment containing novel heterocyclic molecule has been developed through a carbanion induced transformation of suitably functionalized 2H-pyran-2-ones, benzo[h]chromene and thiochromeno[4,3-b]pyrans. Due to the presence of fluorescence, we report their prime application metal sensor as off/on switching in ferric ions. 相似文献
17.
Synthesis of substituted pyrrolo[1,2-a]pyrazines and pyrazino[1,2-a]indoles from the Morita-Baylis-Hillman derivatives of acrylates via saponification followed by Curtius reaction is described. 相似文献
18.
用正丁胺作为碳源,采用射频辉光放电制备碳膜,选用激光染料R6G和聚乙二醇混合液作为蒸气源,采用单源热蒸发,在蒸发室与染料同时沉积得到混合膜,用拉曼光谱和红外光谱分析了碳膜的结构和键合方式,分析表明:碳膜中存在胺基团和氢原子.混合膜的荧光谱测量结果表明,认为正丁胺对染料荧光谱的影响是因为胺基和氢原子的存在. 相似文献
19.
An efficient tandem approach for the selective synthesis of 4,5-dihydroimidazo[1,5-a]quinoxalines 6a–g and imidazo[1,5-a]quinoxalines 7a–h by the reaction of 2-imidazolyl anilines 4a–c with aryl aldehydes 5a–k under mild reaction conditions is described. Introduction of electron releasing alkyl groups in substrates 4a–b was found to be instrumental for the success of the reaction. 相似文献
20.
The Diels-Alder reactivity of 1,2-heteroborines (H4C4B(H)X, X?=?NH, PH, AsH; O, S, Se) has been computationally explored by means of Density Functional Theory (DFT) calculations. The influence of the HB?=?X fragment on the reactivity of the system has been quantitatively analyzed in detail by means of the so-called Activation Strain Model (ASM) of reactivity. It is found that the interaction between these species and the dienophile is significantly stronger than that computed for their all-carbon isoelectronic counterpart, benzene. In addition, the strain energy plays a key role in the observed reactivity trends. The role of the aromaticity strength of these heteroarenes on the reactivity is also assessed. 相似文献