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Influence of Solvent on the Pore Structure and Activity of Pt-Sn/Alumino- Silicate Catalysts 溶剂对Pt-Sn/铝硅酸盐催化剂孔隙结构和活性的影响
Pub Date : 2009-07-03 DOI: 10.2174/1876214X00902010110
M. Riad, S. Mikhail
Kaolinite supported bimetallic Pt-Sn catalysts were prepared via impregnation technique using different sol- vents, water, ethanol and acetone. The catalysts were characterized by X-ray diffraction pattern and temperature pro- grammed reduction techniques. Surface area and pore size distribution were determined by nitrogen physisorption tech- nique. The activities of the catalysts were measured toward n-pentane isomerization reaction in a pulse micro-catalytic re- actor operated under atmospheric pressure and at reaction temperature ranged from 200-450 o C. The results indicated that the selectivity of the Pt-Sn/kaolinite catalysts toward iso-pentane formation decreased from ethanol to acetone and then to water. Pore size distribution and diffusion coefficient of reactant and products are responsible for the high selectivity of Pt-Sn /kaolinte (ethanol) catalyst towards iso-pentane formation.
采用浸渍法制备了高岭石负载型Pt-Sn双金属催化剂,浸渍剂为不同的溶剂孔、水、乙醇和丙酮。用x射线衍射图和程序升温还原技术对催化剂进行了表征。采用氮气物理吸附法测定了其比表面积和孔径分布。在常压下、反应温度200 ~ 450℃的脉冲微催化反应器中测定了催化剂对正戊烷异构化反应的活性。结果表明,Pt-Sn/高岭石催化剂对异戊烷的选择性从乙醇→丙酮→水依次下降。Pt-Sn /高岭石(乙醇)催化剂对异戊烷形成具有高选择性,反应物和生成物的孔径分布和扩散系数是主要原因。
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引用次数: 1
Positive Effects of Ionic Liquids in the Oxidative Cleavage of vic-diols Catalyzed by Mn(III) Complexes 离子液体在锰(III)配合物催化维二醇氧化裂解中的积极作用
Pub Date : 2009-06-16 DOI: 10.2174/1876214X00902010101
D. Fernández, S. Riaño, L. Fadini
The obtaining of aldehydes or ketones through oxidative cleavage of vicinal diols requires the use of a catalyst. In this work we present the positive effects of ionic liquids in the homogeneous oxidative cleavage of ethylenglycol, pinacol, benzopinacol and hydrobenzoin, catalyzed by Mn(salen) complexes. The catalyst dissolved in ionic liquids allows high efficiency (yield up to 99% with air as oxidant), low environmental impact and, in addition, it is possible to recycle. In order to understand the role of the catalyst and of the ionic liquids, DFT studies were performed and a possible catalytic cycle is presented.
通过邻二醇的氧化裂解得到醛或酮需要使用催化剂。在这项工作中,我们提出了离子液体在Mn(salen)配合物催化的乙乙二醇、品那考、苯并匹那考和对苯并安息香的均相氧化裂解中的积极作用。溶解在离子液体中的催化剂效率高(在空气作为氧化剂的情况下收率可达99%),对环境的影响小,此外,还可以回收利用。为了了解催化剂和离子液体的作用,进行了DFT研究,并提出了一个可能的催化循环。
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引用次数: 2
A New Method for the Preparation of Oxazaborolidine Catalyst In Situ Using 1,2-Aminoalcohol, Sodium Borohydride, and Diiodomethane for the Asymmetric Reduction of Prochiral Ketones and N-Substituted Imines 1,2-氨基醇、硼氢化钠和二碘甲烷原位制备恶唑硼烷催化剂的新方法用于前手性酮和n -取代亚胺的不对称还原
Pub Date : 2009-06-16 DOI: 10.2174/1876214X00902010096
Kettouche Hichem Sadrik, Djerourou Abdel Hafid
An oxazaborolidine catalyst is readily prepared in situ at room temperature in THF using 1,2-aminoalcohols and borane generated from sodium borohydride/CH2I2 reagent system. The oxazaborolidine/BH3 reagent system prepared in this way is useful for the reduction of prochiral ketones and N-substituted imines to the corresponding alcohols and amines with moderate to good enantiomeric excesses.
以硼氢化钠/CH2I2试剂体系生成的1,2-氨基醇和硼烷为原料,在室温下原位制备了恶唑硼烷催化剂。用这种方法制备的恶唑硼烷/BH3试剂体系可用于将前手性酮和n -取代亚胺还原为相应的醇和胺,具有中等至良好的对映体过量。
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引用次数: 3
Microwave Polyol Synthesis of Pt/C Catalyst and its Application to Hydrolysis of Sodium Borohydride 微波多元醇合成Pt/C催化剂及其在硼氢化钠水解中的应用
Pub Date : 2009-05-22 DOI: 10.2174/1876214X00902010092
Dongyan Xu, Haizhen Wang, P. Dai, Qingguo Ye
XC-72 carbon supported Pt catalyst was prepared by using a microwave heated ethylene glycol method and characterized by transmission electron microscopy (TEM) and X-ray diffraction (XRD). For comparison, the same Pt/XC- 72 catalyst was also prepared by conventional heated ethylene glycol method. TEM image showed that microwave syn- thesized Pt nanoparticles were uniformly dispersed on the surface of carbon and had a narrow size distribution. The aver- age particle sizes of Pt nanoparticles synthesized with microwave irradiation and conventional heating method are 2.7 and 3.7 nm, respectively. The Pt/C catalysts exhibited four diffraction peaks that are indexed to the {1 1 1}, {2 0 0}, {2 2 0}, and {3 1 1} planes of Pt. Their catalytic performances were evaluated by hydrolysis of sodium borohydride. The micro- wave synthesized Pt/XC-72 catalyst exhibited higher catalytic activity than that synthesized with conventional heated eth- ylene glycol method.
采用微波加热乙二醇法制备了XC-72碳载Pt催化剂,并用透射电子显微镜(TEM)和x射线衍射仪(XRD)对催化剂进行了表征。为了比较,采用传统的加热乙二醇法制备了相同的Pt/XC- 72催化剂。TEM图像显示,微波合成的Pt纳米颗粒均匀分布在碳表面,尺寸分布较窄。微波辐照法制备的铂纳米粒子平均粒径为2.7 nm,常规加热法制备的铂纳米粒子平均粒径为3.7 nm。Pt/C催化剂具有4个衍射峰,分别对应于Pt的{1 1 1}、{2 0 0}、{2 0 0}和{3 1 1}平面。微波合成的Pt/XC-72催化剂比传统的加热乙炔乙二醇法合成的催化剂具有更高的催化活性。
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引用次数: 7
Cataluminescence and Catalysis Properties of CO Oxidation Over Porous Network of ZrO2 Nanorods Synthesized by a Bio-Template 生物模板合成ZrO2纳米棒多孔网络上CO氧化的催化发光及催化性能
Pub Date : 2009-05-08 DOI: 10.2174/1876214X00902010086
Teng Fei, Zhu Yongfa, He Gang, Gao Guizhi, Meng Dennis Desheng
A network of ZrO2 nanorods was prepared using the porous biomembranes as templates. The sample was char- acterized by SEM, XRD and nitrogen physicosorption isotherm. ZrO2 nanoparticles were also prepared with a hydrother- mal method in order to compare with this network. The results showed that after being calcined at 800 o C for 24 h, a vol- ume contraction of ZrO2 nanorod network occurred accompanied by a phase transformation of tetragonal-to-monoclinic ZrO2; but the nanoparticles have grown into the large microparticles; as a result, ZrO2 nanorod network has a higher BET area (45.7 m 2 g -1 ) and a larger pore volume (0.20 cm 3 g -1 ). The calcined network showed a higher cataluminescence (CL) intensity of CO oxidation and a higher combustion activity than the calcined particles, which was ascribed its high surface area, as well as advanced pores.
以多孔生物膜为模板制备了ZrO2纳米棒网络。采用SEM、XRD和氮气物理吸附等温线对样品进行了表征。为了与该网络进行比较,还采用水热法制备了纳米ZrO2。结果表明:在800℃下煅烧24 h后,ZrO2纳米棒网络发生体积收缩,ZrO2由四边形向单斜晶相转变;但是纳米颗粒已经长成了大的微粒;因此,ZrO2纳米棒网络具有更高的BET面积(45.7 m 2 g -1)和更大的孔隙体积(0.20 cm 3 g -1)。煅烧网络比煅烧颗粒表现出更高的CO氧化催化发光强度和更高的燃烧活性,这归因于其高表面积和超前孔隙。
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引用次数: 2
Characterization of Catalyst-Supported Dielectric Barrier Discharge Reactor 催化剂负载介质阻挡放电反应器的表征
Pub Date : 2009-04-28 DOI: 10.2174/1876214X00902010079
Yao Shui-liang, Yamamoto Shin, Kodama Satoshi, Mineo Chieko, F. Yuichi
The discharge properties and chemical reactions in plasma discharges using dielectric (alumina Al2O3) barrier discharge (DBD) reactors supported with Fe2O3 and TiO2 catalyst layers have been characterized. Ozone (O3) was used as a probe substance to monitor the chemical reactions driven by plasma discharges. The light emission from discharge gaps of the catalyst-supported DBD reactors due to plasma discharges was evaluated, using a monochromator equipped with a high dynamic range streak camera. It has been found that the catalyst layers of Fe2O3 and TiO2 do not obviously influence plasma discharges and O3 generation. Light emission from the discharge gaps of the catalyst-supported DBD reactors is different possibly due to the difference in light absorption and scattering by catalyst layers. The mechanism of catalysis effect on PM oxidative removal over Fe2O3 has been proposed, where Fe2O3 layer has the highest light absorption effect compared with that of TiO2 and Al2O3.
研究了Fe2O3和TiO2催化剂层负载的介质(氧化铝Al2O3)阻挡放电(DBD)反应器在等离子体放电中的放电特性和化学反应。臭氧(O3)作为探测物质监测等离子体放电驱动的化学反应。利用配备高动态范围条纹相机的单色仪,对等离子体放电引起的催化剂支撑DBD反应器放电间隙的光发射进行了评估。研究发现,Fe2O3和TiO2的催化剂层对等离子体放电和O3的生成没有明显影响。催化剂负载的DBD反应器放电间隙的光发射不同,可能是由于催化剂层对光的吸收和散射不同。提出了Fe2O3层对PM氧化脱除的催化作用机理,其中Fe2O3层的光吸收效果比TiO2和Al2O3层的光吸收效果最好。
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引用次数: 10
Stereoselective Aminomethylation of m-Cresol with Chiral Amine Mediated by 4 A0 Molecular Sieves Under Neat Conditions 整洁条件下4 A0分子筛介导间甲酚与手性胺的立体选择性氨基甲基化反应
Pub Date : 2009-04-28 DOI: 10.2174/1876214X00902010054
M. Gholizadeh
A minomethylation at ortho position with respect to hydroxyl group of mcresol in presence carefully dried 4A molecular sieves under neat conditions. One pot, two component,Mannich reaction of m-cresol with imine at 600C temperature under solvent free conditions affords the corresponding aminomethylated products in good yields, with moderate stereoselectivity.
在4A分子筛的整洁条件下,对甲酚羟基进行邻位甲基化。间甲酚与亚胺在无溶剂条件下,在600℃温度下进行一锅双组份Mannich反应,得到相应的胺甲基化产物,收率高,立体选择性适中。
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引用次数: 0
A Simple Preparation Route to Palladium Nanoparticles Catalyst from Decomposition of Supported [Pd(lysine·HCl)(Cl)2] Complex 负载型[Pd(赖氨酸·HCl)(Cl)2]配合物分解制备钯纳米颗粒催化剂的简单方法
Pub Date : 2009-04-24 DOI: 10.2174/1876214X00902010066
Hao Yu-zhi, Zhang Yu-long, Wang Li-hua, Ju Xiao-Yan
The supported palladium nanoparticles catalyst with uniform-sized Pd particles distribution and without nitro- gen or chlorine atoms present in catalyst was prepared by calcination of the supported (Pd(lysine·HCl)(Cl)2) complex as precursor and characterized by TEM. Moreover the supported (Pd(lysine·HCl)(Cl)2) complex was from cation exchanging (Pd(lysine·HCl)(Cl)2) complex with inorganic support. The hydrogenation characteristic of supported Pd nanoparticles catalyst was evaluated by using benzoic acid.
以负载型(Pd(赖氨酸·盐酸)(Cl)2)配合物为前驱体,煅烧制备了尺寸均匀、不含氮和氯原子的负载型钯纳米催化剂,并用透射电镜对其进行了表征。Pd(赖氨酸·HCl)(Cl)2配合物是由Pd(赖氨酸·HCl)(Cl)2与无机载体阳离子交换形成的配合物。采用苯甲酸对负载型钯纳米催化剂的加氢特性进行了评价。
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引用次数: 1
Kinetics and Mechanism of Oxidation of D-Galactose by Chromium(VI) in Presence of 2,2 ´ -Bipyridine Catalyst in Aqueous Micellar Media 在2,2´-联吡啶催化剂存在下,水胶束介质中铬(VI)氧化d -半乳糖的动力学及机理
Pub Date : 2009-04-24 DOI: 10.2174/1876214X00902010071
Bayen Ruhidas, K. DasAsim
In aqueous H2SO4 media, the chromic acid oxidation of D-galactose in the presence and absence of 2,2 ´ - bipyridine (bpy) has been carried out under the conditions, (D-galactose)T >> (Cr(VI))T at different temperatures. The monomeric species of Cr (VI) has been found to be kinetically active in the absence of bpy whereas in the bpy-catalysed path, the Cr(VI) -bpy complex has been suggested as the active oxidant. In the bpy-catalysed path, Cr(VI)-bpy complex receives a nucleophilic attack by the substrate to form a ternary complex, which subsequently experiences a redox decomposition (through 2e transfer) at the rate-determining step leading to the product lactone and Cr(IV)-bpy complex. Then the Cr(IV)-bpy complex participates in faster steps in further oxidation of D- galactose and ultimately it is converted into Cr(III)-bpy complex. In the uncatalysed path, Cr(VI)-substrate ester experiences acid catalysed redox decomposition (2e-transfer) at the rate determining step. The uncatalysed path shows second order dependence on (H + ) while the bpy- catalysed path shows a first order dependence on (H + ). Both the uncatalysed path and bpy-catalysed path show the first order dependence on both (D-galactose)T and (Cr(VI))T. The bpy-catalysed path is first order in (bpy)T. These observations remain unaltered in the presence of externally added surfactants. Effect of the surfactants like N-cetylpyridinium chloride (CPC, a cationic surfactant) and sodium dodecyl sulfate (SDS, an anionic surfactant), on both the uncatalysed and bpy- catalysed paths has been studied. CPC inhibits both the uncatalysed and bpy-catalysed path, while SDS accelerates the reactions. In the catalysed path, cationic Cr(VI)-bpy complex is the reactive species which is attracted by the anionic micellar head groups of SDS but repelled by the cationic micellar head groups of CPC. The neutral substrate is accumulated in the Stern layer of both types of micelles. Thus the observed micellar effects have been explained by considering the hydrophobic and electrostatic interactions between the reactants and surfactants in terms of the proposed mechanism.
在H2SO4水溶液中,在2,2´-联吡啶(bpy)存在和不存在的条件下,在不同温度下(d -半乳糖)T > (Cr(VI))T的条件下,进行了d -半乳糖的铬酸氧化反应。单体Cr(VI)在不含bpy的情况下具有动力学活性,而在bpy催化过程中,Cr(VI) -bpy络合物被认为是活性氧化剂。在bpy催化途径中,Cr(VI)-bpy配合物受到底物的亲核攻击,形成三元配合物,随后在速率决定步骤经历氧化还原分解(通过2e转移),导致产物内酯和Cr(IV)-bpy配合物。然后,Cr(IV)-bpy配合物参与D-半乳糖进一步氧化的更快步骤,并最终转化为Cr(III)-bpy配合物。在非催化途径中,Cr(VI)-底物酯在速率决定步骤经历酸催化氧化还原分解(2e-转移)。未催化路径对(H +)有二级依赖性,而bpy-催化路径对(H +)有一级依赖性。非催化途径和半催化途径对(d -半乳糖)T和(Cr(VI))T均表现出一级依赖性。bpy催化的路径在(bpy)T中是一级的。在外部添加表面活性剂的情况下,这些观察结果保持不变。研究了阳离子表面活性剂n -十六烷基吡啶氯化钠(CPC)和阴离子表面活性剂十二烷基硫酸钠(SDS)对非催化和正催化反应路径的影响。CPC对未催化和催化反应均有抑制作用,而SDS对反应有加速作用。在催化过程中,阳离子Cr(VI)-bpy配合物为活性物质,被SDS的阴离子胶束头基团吸引,而被CPC的阳离子胶束头基团排斥。中性底物积聚在两种胶束的尾层中。因此,观察到的胶束效应可以通过考虑反应物和表面活性剂之间的疏水和静电相互作用来解释。
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引用次数: 10
Waugh Type Enneamolybdomanganate(IV) Catalyzed Synthesis of Polyhydrquinoline Through Hantzsch Multi-Component Condensation Waugh型内聚钼锰酸酯(IV)催化Hantzsch多组分缩合合成多羟基喹啉
Pub Date : 2009-04-21 DOI: 10.2174/1876214X00902010061
A. Supale, G. Gokavi
An efficient one pot coupling of aldehydes, dimedone, ammonium acetate and ethyl acetoacetate by using cata- lytic amount of enneamolybdomanganate(IV) is reported. Various polyhydroquinoline derivatives have been prepared in high yields and comparatively less reaction time.
本文报道了一种用乙酸铵、二美酮、乙酸铵和乙酰乙酸乙酯等四种醛类化合物的高效一锅偶联反应。以较高的收率和较短的反应时间制备了各种聚对苯二酚衍生物。
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引用次数: 5
期刊
The Open Catalysis Journal
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