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Chinese Journal of Catalysis
2011, Vol. 32, No. 12
Online: 21 December 2011


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Li and coworkers in their Article on pages 1790–1802 report a novel route for the selective production of linear α-olefins of various chain lengths by Fischer-Tropsch synthesis from syngas. A higher α-olefin selectivity was obtained by preventing olefin secondary reactions by the use of a polar liquid phase. The α-olefin content was almost independent of carbon num-ber for hydrocarbons of different lengths.

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Table of Contents for Vol. 32 No. 12 2011, 32 (12):  0-0.  Abstract ( 1192 )   PDF (1135KB) ( 805 )

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Contents for Volume 32 (2011) 2011, 32 (12):  1-1.  Abstract ( 1154 )   [Full Text(HTML)] () PDF (863KB) ( 1159 )

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Author Index for Volume 32 (2011) 2011, 32 (12):  2-2.  Abstract ( 1152 )   [Full Text(HTML)] () PDF (291KB) ( 754 )

Research Briefing

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Mesoporous Carbon Supported Pd Catalysts for the Hydrogenation of β-Sitosterol to β-Sitostanol CHEN Hui, DAI Le, XIE Jian-Xin, BAI Zhi-Ping, JIA Min-Hui, SHEN Jian-Yi 2011, 32 (12):  1777-1781.  DOI: 10.1016/S1872-2067(10)60294-X Abstract ( 2764 )   [Full Text(HTML)] () PDF (546KB) ( 940 )   Supported palladium catalysts on mesoporous carbons (CMC) were prepared by liquid phase reduction and used for the hydrogenation of β-sitosterol to β-sitostanol. Compared to Pd/AC (active carbon), the Pd/CMC catalysts showed significantly higher activity for the hydrogenation of large molecules due to their larger pore size.

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Oxidative Carbonylation of 2-Amino-1-alkanols Catalyzed by Cross-Linked Polymer Supported Palladium in Water WANG Yan, LIU Jian-Hua, XIA Chun-Gu 2011, 32 (12):  1782-1786.  DOI: 10.1016/S1872-2067(11)60328-8 Abstract ( 2613 )   [Full Text(HTML)] () PDF (1018KB) ( 801 )   Employing palladium supported on polymeric monolith containing ionic liquid as an efficient heterogeneous catalyst, the oxidative carbonylation of 2-amino-1-alkanols could be successfully carried out, affording the corresponding 2-oxazolidinones in good to excellent yields in pure water without excessive iodine-containing promoter. The catalyst was reused up to five cycles without significant loss of its catalytic activity.

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N-Hydroxyquinolinimide Copper Complex Catalyzing Selective Oxidation of Hydrocarbon ZHANG Qiao-Hong, CHEN Chen, MA Hong, GAO Jin, XU Jie, XIA Chun-Gu 2011, 32 (12):  1787-1789.  DOI: 10.3724/SP.J.1088.2011.10839 Abstract ( 2351 )   [Full Text(HTML)] () PDF (409KB) ( 791 )   A N-hydroxyquinolinimide copper complex was synthesized and its composition and structure were characterized by elemental analysis and FT-IR. This complex is an efficient catalytic system for selective oxidation of hydrocarbons such as cyclohexene, ethylbenzene, etc., and higher activity can be obtained under mild conditions.

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Product Distribution of Fischer-Tropsch Synthesis in Polar Liquids GAO Jun-Hu, WU Bao-Shan, ZHOU Li-Ping, YANG Yong, HAO Xu, XU Yuan-Yuan, LI Yong-Wang 2011, 32 (12):  1790-1802.  DOI: 10.1016/S1872-2067(10)60285-9 Abstract ( 2895 )   [Full Text(HTML)] () PDF (718KB) ( 1705 )   The effect of using polar liquid as the reaction medium for Fischer-Tropsch synthesis on the product distribution was studied. The experiments were performed with an industrial iron-based catalyst in a batch autoclave reactor with different liquid phases (polyethylene glycol 400, polyethylene glycol 600, 1,4-butanediol, and glycol). The reaction conditions were temperature of 200–240 °C, initial H2/CO molar ratios of 1.00–2.03, catalyst particle sizes of 20–40 mesh and > 150 mesh, and reaction time of 24–144 h. The α-olefin selectivity was significantly increased to more than 70% and was almost independent of carbon number with all the polar liquids. Most of the hydrocarbon distribution were not of the ideal Anderson-Schulz-Flory pattern and could not be explained by the mechanism of olefin readsorption and secondary reactions. The chain growth probability α was larger than 0.85 for all conditions, and it was slightly influenced by changes of reaction conditions, liquid, and reaction time. There was product separation during reaction in this catalytic system, which meant that it did not have the problem of separating the catalyst from the wax product that traditional slurry reactors have. The result suggested new opportunities for the selective production of linear α-olefins and for mechanistic investigations of Fischer-Tropsch synthesis.

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Ceria Modified MnOx/TiO2-Pillared Clays Catalysts for Selective Catalytic Reduction of NO with NH3 at Low Temperature SHEN Bo-Xiong, YAO Yan, MA Hong-Qing, LIU Ting 2011, 32 (12):  1803-1811.  DOI: 10.1016/S1872-2067(10)60269-0 Abstract ( 2748 )   [Full Text(HTML)] () PDF (646KB) ( 1175 )   Titania-pillared clays (TiO2-PILC) were synthesized by ion exchange and manganese was introduced as the active phase. The catalytic behavior of the xMn/TiO2-PILC catalysts was studied for the low-temperature selective catalytic reduction (SCR) of NO with NH3. A series of Ce-doped 8%Mn-yCe/TiO2-PILC catalysts were prepared and evaluated for their performance in the low-temperature SCR of NO with NH3, their resistance to water vapor (H2O), and their resistance to sulfur dioxide (SO2). It was found that the NO conversion properties of the 8%Mn/TiO2-PILC catalysts could be significantly improved by adding Ce and all the catalysts gave high resistance to H2O but were sensitive to SO2. The catalyst with a Ce loading of 2% gave 95% NO conversion at 220 °C and exhibited a moderate SO2-poisoning resistance compared with the other catalysts. X-ray diffraction, N2 adsorption-desorption, temperature-programmed desorption of NH3, X-ray photoelectron spectroscopy, and temperature-programmed reduction of H2 were used to characterize the properties of the catalysts. The addi-tion of Ce improved the diffusion of Mn on the surfaces of the catalysts, which enhanced the surface acidity and improved the reduction properties of the catalysts and these were the main influencing factors for the low-temperature SCR.

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Preparation of Immobilized Chromium Schiff Base Complexes and Their Catalytic Performance for Cyclohexene Epoxidation WANG Xiao-Li, WU Gong-De, WANG Fang, WEI Wei, SUN Yu-Han 2011, 32 (12):  1812-1821.  DOI: 10.1016/S1872-2067(10)60272-0 Abstract ( 2445 )   [Full Text(HTML)] () PDF (562KB) ( 991 )   Three typical amino acid Schiff base chromium(III) complexes immobilized on MCM-41 were prepared and characterized by various physico-chemical methods such as Fourier transform infrared spectroscopy, ultraviolet-visible spectroscopy, X-ray powder diffraction, N2 sorption, and elemental analysis. The obtained immobilized complexes were effective catalysts for the epoxidation of cyclohexene with 30% hydrogen peroxide and they exhibited significantly enhanced catalytic performance compared with their corresponding homogeneous analogues. Under optimal reaction conditions the highest conversion of cyclohexene was 52.6% with 73.5% epoxide selectivity. In addition, the catalytic activity was retained after recycling 6 times.

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Preparation of Sodium Tantalate with Different Structures and Its Photocatalytic Activity for H2 Evolution from Water Splitting HUANG Lang-Huan, CHAN Qi-Zhong, ZHANG Bin, WU Xiao-Jing, GAO Peng, JIAO Zi-Bin, LIU Ying-Liang 2011, 32 (12):  1822-1830.  DOI: 10.1016/S1872-2067(10)60286-0 Abstract ( 3235 )   [Full Text(HTML)] () PDF (618KB) ( 4697 )   Sodium tantalate photocatalysts with a perovskite structure (NaTaO3), a pyrochlore structure (Na2Ta2O6), and a nano-heterojunction (NaTaO3/Na2Ta2O6) structure were controllably synthesized using the hydrothermal method. Sodium carbonate, sodium stearate, and sodium acetate were used as precursors, respectively. The physical properties of the as-prepared samples were characterized by X-ray diffraction, scanning electron microscopy, high resolution transmission electron microscopy, ultraviolet visible diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, and photoluminescence spectroscopy. The effects of the sodium precursor on the structure of sodium tantalate are discussed. The photocatalytic results indicated that the activity for the H2 evolution half-reaction from water splitting was in the following order: NaTaO3/Na2Ta2O6 > NaTaO3 > Na2Ta2O6. The highest photocatalytic activity of NaTaO3/Na2Ta2O6 can be attributed to heterojunction formation within the nanoparticles, which significantly enhanced the separation of the electron-hole pairs.

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Glycerol Oxidation with Oxygen over Bimetallic Pt-Bi Catalysts under Atmospheric Pressure LIANG Dan, CUI Shi-Yu, GAO Jing, WANG Jun-Hua, CHEN Ping, HOU Zhao-Yin 2011, 32 (12):  1831-1837.  DOI: 10.1016/S1872-2067(10)60289-6 Abstract ( 2565 )   [Full Text(HTML)] () PDF (731KB) ( 1102 )   A series of bimetallic Pt-Bi catalysts with a constant platinum content of 5.0 wt% and a varied bismuth content (3.0–7.0 wt%) supported on active carbon were prepared and used for glycerol oxidation with oxygen under atmospheric pressure. The bimetallic Pt-Bi/C was efficient for the selective oxidation of glycerol to dihydroxyacetone (DIHA) and the selectivity for DIHA reached 49.0% at a 91.5% conversion of glycerol over the 5%Pt-5%Bi/C catalyst. X-ray diffraction and transmission electron microscopy analysis revealed that the specially configured Pt-Bi nanoparticles in 5%Pt-5%Bi/C were highly dispersed (3.8 nm) over the active carbon support, which is proposed to contribute to the improved performance.

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Fabrication of a TiO2/Au Nanorod Array for Enhanced Photocatalysis LU Ying, CHEN Shuo, QUAN Xie, YU Hong-Tao 2011, 32 (12):  1838-1843.  DOI: 10.1016/S1872-2067(10)60288-4 Abstract ( 2784 )   [Full Text(HTML)] () PDF (843KB) ( 1146 )   A highly ordered TiO2/Au nanorod array was successfully fabricated by direct current electrodeposition and subsequent spin-coating. Scanning electron microscopy and transmission electron microscopy images revealed that the TiO2 film completely covered the surface of the Au nanorods, which resulted in TiO2 shell Au core nanorods. X-ray diffraction patterns revealed that the TiO2 film was anatase with preferential orientation in the (101) plane. UV-Vis diffuse reflectance spectra showed a shift in the absorption edge toward the visible region because of the formation of a Schottky junction between Au and TiO2. A new absorption peak that ranged from 400 to 800 nm appeared because of the localized surface plasmon resonance of the Au nanorod arrays. For the photocatalytic degradation of rhodamine B under UV light irradiation, the TiO2/Au nanorod array exhibited excellent photocatalytic activity and its kinetic constant was 2.0 times that of pristine TiO2 and 1.3 times that of a TiO2/Au film. The enhanced photocatalysis was attributed to the high surface volume ratio, an improved UV light response, efficient separation, and the convenient migration of photogenerated charge carriers because of the one-dimensional nanorod structure and the Schottky junction between Au and TiO2. This work could provide new insights into the fabrication of a high performance photocatalyst and thus facilitate practical environmental applications.

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Synthesis of Nickel Hexacyanoferrate Nanoparticles and Their Potential as Heterogeneous Catalysts for the Solvent-Free Oxidation of Benzyl Alcohol Shah R. ALI, Prakash CHANDRA, Mamta LATWAL, Shalabh K. JAIN, Vipin K. BANSAL, Sudhanshu P. SINGH 2011, 32 (12):  1844-1849.  DOI: 10.1016/S1872-2067(10)60292-6 Abstract ( 2690 )   [Full Text(HTML)] () PDF (211KB) ( 1992 )   Nickel hexacyanoferrate nanoparticles were synthesized and characterized using elemental analysis, thermal analysis, infrared spectroscopy, and X-ray diffraction. A FE-SEM image of the nickel hexacyanoferrate showed that it consists of nearly spherical particles with sizes ranging from 30 to 70 nm. The synthesized material was found to be a heterogeneous catalyst useful for the solvent-free oxidation of benzyl alcohol with H2O2 as an oxidant. A 36% conversion of benzyl alcohol to benzaldehyde was achieved under optimized reaction conditions using specific parameters such as the amount of catalyst, the temperature, the benzyl alcohol to H2O2 molar ratio, and the reaction time.

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Cobalt Nanoparticles Promoted Highly Efficient One Pot Four-Component Synthesis of 1,4-Dihydropyridines under Solvent-Free Conditions Javad SAFARI, Sayed Hossein BANITABA, Shiva DEHGHAN KHALILI 2011, 32 (12):  1850-1855.  DOI: 10.1016/S1872-2067(10)60295-1 Abstract ( 2579 )   [Full Text(HTML)] () PDF (1065KB) ( 1335 )   A straightforward and general method has been developed for the synthesis of C5-unsubstitiuted 1,4-dihydropyridines by a reaction using dimedone, acetophenone, aromatic aldehydes, and ammonium acetate in the presence of a catalytic amount of Co nanoparticles as a heterogeneous and eco-friendly catalyst with high catalytic activity at room temperature under solvent-free conditions. This catalyst is easily separated by magnetic devices and can be reused without any apparent loss of activity for the reaction. In addition, it is very interesting that when using Co nanoparticles as a catalyst, spatially-hindered aldehydes such as 2-methoxy-, 2-fluoro-, and 2-chloro-aldehydes are suitable for this reaction.

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Pt-Ir-SnO2/C Electrocatalysts for Ethanol Oxidation in Acidic Media ZHAO Lian-Hua, Shigenori MITSUSHIMA, Akimitsu ISHIHARA, Koichi MATSUZAWA , Ken-ichiro OTA 2011, 32 (12):  1856-1863.  DOI: 10.1016/S1872-2067(10)60297-5 Abstract ( 2731 )   [Full Text(HTML)] () PDF (737KB) ( 1077 )    A series of Pt-Ir-SnO2/C catalysts were synthesized by a modified Bönnemann method. An electrochemical study showed that the Pt-Ir0.07-SnO2/C catalyst had a three times higher ethanol oxidation current and a two times higher CO2 formation selectivity compared with the Pt/C catalyst under an application voltage of 0.5 V vs the RHE at 25 °C. This demonstrates that the Pt-Ir0.07-SnO2/C catalyst is a potentially ideal ethanol oxidation catalyst for direct ethanol fuel cells.

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Silylation of Alcohols and Phenols with Hexamethyldisilazane over Highly Reusable Propyl Sulfonic Acid Functionalized Nanostructured SBA-15 Daryoush ZAREYEE, Rezvaneh ASGHARI, Mohammad A. KHALILZADEH 2011, 32 (12):  1864-1868.  DOI: 10.1016/S1872-2067(10)60300-2 Abstract ( 2404 )   [Full Text(HTML)] () PDF (209KB) ( 1761 )   Various alcohols and phenols were trimethylsilylated in excellent yields using hexamethyldisilazane in the presence of catalytic amounts of environmentally friendly, hydrophobic, highly thermal stable, and completely heterogeneous sulfonic acid functionalized mesostructured SBA-15 in dichloromethane at ambient temperature. Primary, bulky secondary, tertiary, and phenolic hydroxyl functional groups were transformed to the corresponding trimethylsilyl ethers in excellent yields. The simple experimental procedure was accompanied by easy recovery and the catalyst was reusable (at least 18 reaction cycles); these are attractive features of this protocol.

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Flexible Immobilization of Lipase on Hydrophilic and Comblike Polymer Support Containing Epoxy Group QU Wei-Guang, WEI Rong-Qing, HE Bing-Fang, LIU Xiao-Ning, ZHONG Yu, CHEN Xin-Ying 2011, 32 (12):  1869-1874.  DOI: 10.3724/SP.J.1088.2011.10536 Abstract ( 2257 )   [Full Text(HTML)] () PDF (462KB) ( 879 )   A hydrophilic and comblike polymer support PS-acyl-P(acrylamide-co-glycidyl methacrylate) containing epoxy groups for flexible and covalent immobilization of lipase has been prepared by an atom transfer radical polymerization method. The grafting reaction of glycidyl methacylate and hydrophilic acrylamid was initiated from the chloroacetyl groups on the styrene-divinylbenzene copolymer microspheres with CuCl and 2,2′-bipyridine complex as a catalyst. The apparent activity of lipase immobilized on PS-acyl-P(acrylamide-co-glycidyl methacrylate) was 16.6 U/g, and the optimal temperature and pH were 45–55 oC and 8.5 for hydrolysis of p-nitrophenyl palmitate, respectively. The immobilized lipase was stable in the range of pH = 5–10 and at temperature below 80 oC. The operational stability for the immobilized lipase was tested for consecutive hydrolysis of p-nitrophenyl palmitate. The result shows that the immobilized lipase has excellent operational stability. The residual activity of immobilized lipase was 73.5% after used 7 cycles. The activity of immobilized lipase remained 86.8% of the origin after storage at 4 oC for 60 d. Lipase got improved to varying degrees for organic solvent tolerance through immobilization on PS-acyl-P(acrylamide-co-glycidyl methacrylate).

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The Reaction of Aromatic Amines with Propylene Carbonate Catalyzed by Anion-Cation Cooperativity in Ionic Liquids ZHANG Li-Feng, YANG Si-Juan, GAO Guo-Hua 2011, 32 (12):  1875-1879.  DOI: 10.3724/SP.J.1088.2011.10757 Abstract ( 2810 )   [Full Text(HTML)] () PDF (417KB) ( 802 )    Ionic liquid 1-butyl-3-methyl-imidazolium acetate ([bmim]OAc) effectively catalyzed the reaction of aromatic amines with propylene carbonate to 5-methyl-3-aryloxazolidin-2-one. The effects of reaction temperature, time, and catalyst amount were investigated in detail. Under the optimized conditions, the yield of 5-methyl-3-phenyl-oxazolidin-2-one was 99%. The effects of cations and anions in ionic liquids were also studied. The cations play important role for the reaction and the catalytic activity follows the order of 1-butyl-3-methyl-imidazolium ([bmim]) > 1, 2-dimethyl-3-butyl imidazolium ([bmmim]) > 1-butyl-pyridinium ([bpy]), which is consistent with the order of hydrogen bond donor ability. Simultaneously, the anions are also crucial to the reaction and the catalytic activity of imidazolium based ionic liquids follows the order OAc > Cl > Br > BPh4, which is consistent with the order of the hydrogen bond acceptor ability.

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An Overview of Catalysis-Related Papers Published in Acta Physico-Chimica Sinica in the Year 2010 MA Ding 2011, 32 (12):  1880-1884.  DOI: 10.3724/SP.J.1088.2011.11059 Abstract ( 2968 )   [Full Text(HTML)] () PDF (422KB) ( 779 )   In the year 2010, Acta Physico-Chimica Sinica has published 89 papers in the field of catalysis, and the 53 research articles can be divided into 9 topics: petroleum processing, oxidation, hydrogenation, biomass conversion, photo-catalysis, syngas and methanol conversion, theoretical catalysis, electro-catalysis, and environmental catalysis. The papers on the conversion and use of energy were highlighted. It is pointed out that it is the catalysis people’s duty to design cheaper, better and environmentally friendly catalyst/process for more efficient use of tradition/renewable energy resources.