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    Chinese Journal of Catalysis
    2013, Vol. 34, No. 12
    Online: 25 November 2013

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    Zhang and coworkers in their Article on pages 2161–2166 reported an efficient and reusable Suzuki coupling reaction catalyst with an anion exchange resin as support. The catalyst can easily be bifunctionalized via ion exchange process. The obtained bifunctional material can successfully catalyze the Suzuki reaction without the existence of extra base.

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    Table of Contents
    Table of Contents for Vol.34 No.12
    2013, 34 (12):  0-0. 
    Abstract ( 248 )   PDF (5643KB) ( 981 )  
    Contents for Volume 34 (2013)
    2013, 34 (12):  1-1. 
    Abstract ( 208 )   [Full Text(HTML)] () PDF (3632KB) ( 812 )  
    Author Index for Volume 34 (2013)
    2013, 34 (12):  2-2. 
    Abstract ( 183 )   [Full Text(HTML)] () PDF (403KB) ( 510 )  
    Research papers
    Palladium supported on an ion exchange resin for the Suzuki-Miyaura reaction
    Mingming Zhang, Manman Jiang, Changhai Liang
    2013, 34 (12):  2161-2166.  DOI: 10.1016/S1872-2067(12)60698-6
    Abstract ( 372 )   [Full Text(HTML)] () PDF (782KB) ( 739 )  

    A basic anion exchange resin, Amberlite IRA-900, was loaded with Pd(C3H5)(C5H5) by an easy metal-organic chemical vapor deposition (MOCVD) approach to give Pd@IRA-900 catalyst after reduction at room temperature. Ultraviolet-Visible spectroscopy results showed a red shift of the absorption peak of Pd2+ after the Pd precursor was loaded on the resin, indicating that a chemical reaction occurred between the precursor and the support. Pd nanoparticles with 2.6 nm of average size were well dispersed on the support. The Pd@IRA-900 catalyst showed high activity for different kinds of aryl halides in Suzuki-Miyaura coupling reactions under mild and aerobic conditions. Excellent recyclability of Pd@IRA-900 catalyst was also observed in the Suzuki-Miyaura coupling reaction of iodobenzene and phenylboronic acid. A bifunctional catalyst Pd@IRA-900(OH) was synthesized by pretreating the ion exchange resin support with NaOH before Pd loading, which successfully catalyzed the Suzuki-Miyaura reaction of iodobenzene and phenylboronic acid without base under aerobic conditions.

    Aldol condensations of a variety of different aldehydes and ketones under ultrasonic irradiation using poly(N-vinylimidazole) as a new heterogeneous base catalyst under solvent-free conditions in a liquid-solid system
    Nader Ghaffari Khaligh, Taraneh Mihankhah
    2013, 34 (12):  2167-2173.  DOI: 10.1016/S1872-2067(12)60658-5
    Abstract ( 517 )   [Full Text(HTML)] () PDF (315KB) ( 888 )  

    An ultrasound-assisted aldol condensation reaction has been developed for a range of ketones with a variety of aromatic aldehydes using poly(N-vinylimidazole) as a solid base catalyst in a liquid-solid system. The catalyst can be recovered by simple filtration and reused at least 10 times without any significant reduction in its activity. The reaction is also amenable to the large scale, making the procedure potentially useful for industrial applications.

    Highly selective and stable CsPW/Nb2O5 catalysts for dehydration of glycerol to acrolein
    Rong Liu, Tiefeng Wang, Chang Liu, Yong Jin
    2013, 34 (12):  2174-2182.  DOI: 10.1016/S1872-2067(12)60666-4
    Abstract ( 1527 )   [Full Text(HTML)] () PDF (492KB) ( 806 )  

    Acrolein production by gas-phase dehydration of glycerol at 300 ℃, catalyzed by a Cs+-substituted Keggin-type phosphotungstate, Cs2.5H0.5PW12O40 (CsPW), supported on Nb2O5 was investigated. The catalysts were characterized using N2 adsorption-desorption, X-ray diffraction, Fourier-transform infrared and Raman spectroscopies, and NH3 temperature-programmed desorption. It was demonstrated that Lewis acid sites were responsible for byproduct formation, and that Brönsted acid sites of medium strength were the active sites for acrolein production by glycerol dehydration. The acidity of the supported CsPW was affected by the calcination temperature and CsPW loading. The CsPW was well dispersed on Nb2O5 at loadings ≤20 wt%, and the strong acid sites of bulk CsPW were converted to selective medium acid sites. The CsPW catalyst with 20% of CsPW loading calcined at 500 ℃ gave 96% of glycerol conversion and 80% of acrolein selectivity, and there was no significant deactivation in 10 h. The catalyst with a 20% decrease in activity was regenerated by simple coke burning with air at 500 ℃.

    An outstanding Cr-doped catalyst for selective oxidation of propane to acrylic acid
    Aixin Xu, Yang Wang, Hanqing Ge, Shu Chen, Yanhua Li, Weimin Lu
    2013, 34 (12):  2183-2191.  DOI: 10.1016/S1872-2067(12)60671-8
    Abstract ( 257 )   [Full Text(HTML)] () PDF (592KB) ( 612 )  

    The catalytic performance of active MoVTeNbOx catalysts containing an M1 phase in the partial oxidation of propane to acrylic acid (AA) was greatly improved when an optimal amount of Cr was added. The catalyst containing Cr/Nb (molar ratio = 0.002) showed good selectivity (78.3%) and high AA yield (50.7%). The catalysts were characterized using X-ray diffraction, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, O2 and NH3 temperature-programmed desorption, and oxidation of 2-propanol. The relationship between the catalyst structure and catalytic properties was investigated. The results indicated that the amounts of Mo6+, V5+ and Te4+ species on the catalyst surface were adjusted, and oxidation activity of the catalyst increased, as a result of doping with an appropriate amount Cr, which promoted propane activation. The acid strength became weaker, and the number of acid sites on the catalyst surface decreased, which suppressed AA oxidation and improved the selectivity for AA.

    Adsorption isotherms of methanol and dimethyl ether on SAPO-34 measured together with differential adsorption heat measurement
    Yasukazu Kobayashi, Yuxin Li, Yao Wang, Dezheng Wang
    2013, 34 (12):  2192-2199.  DOI: 10.1016/S1872-2067(12)60676-7
    Abstract ( 307 )   [Full Text(HTML)] () PDF (577KB) ( 1059 )  

    Adsorption isotherms of methanol and dimethyl ether on a SAPO-34 zeolite were measured at 25, 60, and 100 ℃. The curves of differential heats of adsorption versus coverage (calorimetric curves) were simultaneously measured with a microcalorimeter, which showed that a simple interpretation of the adsorption isotherms would be incorrect. The calorimetric curves showed sharp drops, and the coverages at which these occurred were taken as the saturation amounts of adsorbed methanol and dimethyl ether on regular sites. However, beyond the saturation coverage, the adsorption isotherms still showed increasing coverages, which were attributed to adsorption on weaker sites, and which should not be used during curve fitting to get the Langmuir parameters of the adsorption isotherm for the regular adsorption sites. In the absence of the calorimetric data, these regions would have been assumed to be part of the adsorption isotherm for the regular adsorption sites, which would be erroneous. To account for the existence of another weaker adsorption site which continued to be populated at high pressures, in addition to the regular adsorption site, we used the dual-site Langmuir equation with the saturation amount on the regular adsorption site obtained from the calorimetric curves. This gave good fits also in the high pressure region where adsorption mainly occurred on the weaker sites.

    Rice husk ash supported FeCl2·2H2O:A mild and highly efficient heterogeneous catalyst for the synthesis of polysubstituted quinolines by Friedländer heteroannulation
    Farhad Shirini, Somayeh Akbari-Dadamahaleh, Ali Mohammad-Khah
    2013, 34 (12):  2200-2208.  DOI: 10.1016/S1872-2067(12)60684-6
    Abstract ( 280 )   [Full Text(HTML)] () PDF (2938KB) ( 640 )  

    Rice husk ash was used as a new, green, and cheap adsorbent for FeCl3. Characterization of the obtained reagent showed that rice husk ash supported FeCl2·2H2O was formed. This reagent is efficient at catalyzing the synthesis of multisubstituted quinolines by the Friedländer heteroannulation of o-aminoaryl ketones with ketones or β-diketones under mild reaction conditions. This methodology allows for the synthesis of a broad range of substituted quinolines in high yields and with excellent regioselectivity in the absence of a solvent.

    Iron-impregnated titania composites for the decomposition of low-concentration aromatic organic pollutants under UV and visible light irradiation
    Wan-Kuen Jo, Joon Yeob Lee
    2013, 34 (12):  2209-2216.  DOI: 10.1016/S1872-2067(12)60688-3
    Abstract ( 198 )   [Full Text(HTML)] () PDF (531KB) ( 693 )  

    Fe-TiO2 photocatalysts with different ratios of Fe to Ti were prepared by a sol-gel process using tetra-n-butyl titanium and iron(Ⅲ) nitrate as Ti and Fe sources, respectively. The photocatalytic function of the prepared composites was examined for the decomposition of low-concentration (0.1 ppm) airborne benzene, toluene, ethyl benzene, and o-xylene (BTEX). The Fe-TiO2 composites were characterized by energy dispersive X-ray spectroscopy, X-ray diffraction, UV-visible spectroscopy, and Fourier transform infrared spectroscopy. The time-series ratios of outlet to inlet concentrations of toluene, ethyl benzene, and o-xylene target chemicals, as determined by the Fe-TiO2 composites under visible light exposure, were lower than or similar to those of the reference TiO2 photocatalyst. Moreover, the time-series ratios of outlet to inlet concentrations of the three compounds, as determined for the Fe-TiO2 composites, increased as the ratio of Fe to Ti increased from 0.001 to 0.010. In contrast, under UV exposure, the time-series ratios of outlet to inlet concentrations of BTEX, determined for the Fe-TiO2 composites, were similar to or higher than those obtained from the reference TiO2 photocatalyst. Fe-TiO2 composites with an optimal Fe to Ti ratio could effectively be applied for the purification of low-concentration aromatic organic pollutants.

    Cu(Ⅱ) salen complex catalyzed synthesis of propargylamines by a three-component coupling reaction
    Mahmood Tajbaksh, Maryam Farhang, Hamid Reza Mardani, Rahman Hosseinzadeh, Yaghoub Sarrafi
    2013, 34 (12):  2217-2222.  DOI: 10.1016/S1872-2067(12)60683-4
    Abstract ( 363 )   [Full Text(HTML)] () PDF (417KB) ( 731 )  

    A one pot three-component coupling reaction of phenylacetylene, aldehyde, and amine derivatives in the presence of Cu(Ⅱ) Salen complex as an efficient heterogeneous catalyst under solvent-free conditions is reported. The catalyst displayed high activity and afforded the corresponding propargylamines in good to excellent yields. This method provides a wide range of substrate applicability. The catalyst was reused several times without significant loss of its catalytic activity.

    Mesoporous LaFeO3 catalysts for the oxidation of toluene and carbon monoxide
    Baozu Gao, Jiguang Deng, Yuxi Liu, Zhenxuan Zhao, Xinwei Li, Yuan Wang, Hongxing Dai
    2013, 34 (12):  2223-2229.  DOI: 10.1016/S1872-2067(12)60689-5
    Abstract ( 390 )   [Full Text(HTML)] () PDF (826KB) ( 831 )  

    Wormhole-like orthorhombic LaFeO3 catalysts (LFO-1 and LFO-2) were prepared using the KIT-6 and SiO2 nanospheres as template, respectively. LFO-1 showed better catalytic activity with T50% and T90% of 155 and 180 ℃ for CO oxidation, and of 200 and 253 ℃ for toluene oxidation at 20000 mL/(g·h). The excellent catalytic performance was associated with its larger surface area (138 m2/g), higher adsorbed oxygen concentration, and better low-temperature reducibility as well as a wormhole-like mesoporous structure.

    Hydrogenolysis of glycerol to propanediols over Cu-MgO/USY catalyst
    Lei Niu, Ruiping Wei, Hui Yang, Xiang Li, Feng Jiang, Guomin Xiao
    2013, 34 (12):  2230-2235.  DOI: 10.1016/S1872-2067(12)60695-0
    Abstract ( 335 )   [Full Text(HTML)] () PDF (772KB) ( 831 )  

    A series of acid-base bifunctional catalysts composed of USY with different Cu and MgO loadings were prepared, characterized, and tested for the hydrogenolysis of glycerol. The USY support retained the Y zeolite structure, and the introduction of MgO enhanced the dispersion of Cu in the support. At 200 ℃, 3.5 MPa H2, 10 h and with a 6% 0.2Cu-MgO/USY catalyst, 83.6% conversion of glycerol with 40% selectivity to 1,2-propanediol (1,2-PDO) and 19.4% selectivity to 1,3-propanediol (1,3-PDO) was achieved.

    Synthesis of dicationic alkyl imidazolium peroxopolyoxotungsten-based phase transfer catalyst and its catalytic activity for olefin epoxidation
    Jianghao Wu, Pingping Jiang, Yan Leng, Yuanyuan Ye, Xiaojie Qin
    2013, 34 (12):  2236-2244.  DOI: 10.1016/S1872-2067(12)60697-4
    Abstract ( 397 )   [Full Text(HTML)] () PDF (685KB) ( 525 )  

    Peroxopolyoxotungsten-based hybrid catalysts modified by dicationic long-chain alkyl imidazolium cations have been synthesized and characterized. The catalytic activity of the catalysts was measured for the epoxidation of olefins with H2O2. These catalysts proved to be high catalytic activity phase transfer catalysts. In particular, for the catalyst [D12min]1.5PW4O24 modified by the dodecyl dicationic imidazolium cation, the conversion of cyclohexene and selectivity for epoxycyclohexane were 97.7% and 96.3%, respectively. After the reaction, the catalyst could be recovered simply by filtration and reused four times. The conversion of cyclohexene and selectivity for epoxycyclohexane were still 72.4% and 97.2%, respectively, after recycling the catalyst four times. In addition, this phase transfer catalyst can be applied to the epoxidation of a wide range of olefins.

    Silica-bonded N-propylpiperazine sodium n-propionate as recyclable catalyst for synthesis of 4H-pyran derivatives
    Khodabakhsh Niknam, Nassim Borazjani, Reza Rashidian, Abbas Jamali
    2013, 34 (12):  2245-2254.  DOI: 10.1016/S1872-2067(12)60693-7
    Abstract ( 284 )   [Full Text(HTML)] () PDF (715KB) ( 808 )  

    Silica-bonded N-propylpiperazine sodium n-propionate (SBPPSP) was found to act as an efficient solid base for the preparation of a series of 4H-benzo[b]pyran derivatives. SBPPSP was used as a recyclable heterogeneous solid base catalyst for the synthesis of 3,4-dihydropyrano[c]chromenes, 2-amino-4H-pyrans, 1,4-dihydropyrano[2,3-c]pyrazoles, and 2-amino-4H-benzo[e]-chromenes via the condensation reaction of dimedone, ethyl acetoacetate, 3-methyl-1-phenyl-1H-pyrazol-5(4H)-one, and α-naphthol, respectively, with aromatic aldehydes and malononitrile in refluxing aqueous ethanol. The heterogeneous solid base showed similar efficiency when reused in consecutive reactions.

    Synthesis of phytosterol esters catalyzed by immobilized lipase in organic media
    Zhenhua Jiang, Min Yu, Liwei Ren, Hua Zhou, Ping Wei
    2013, 34 (12):  2255-2262.  DOI: 10.1016/S1872-2067(12)60700-1
    Abstract ( 252 )   [Full Text(HTML)] () PDF (491KB) ( 847 )  

    Lipase-catalyzed synthesis of phytosterol esters has the advantages of mild reaction conditions and high product purity and yield. However, the activity and stability of enzymes in a non-aqueous phase are generally lower than in an aqueous phase. In this study, a highly efficient synthesis of phytosterol esters was established by using immobilized lipase on a macroporous resin as the catalyst and adding the analogues of lactose during the enzyme catalyzed reaction. In order to facilitate the application of the esterification of phytosterol, the lipases and solvents were screened and the conditions were optimized. In addition, the quantity and type of carbohydrates were investigated, which indicated that immobilized Candida rugosa lipase on NKA (NKA-CRL) was the best catalyst. With a molar ratio of lauric acid to phytosterol of 2, 7.5% enzyme protein added and the reaction carried out at 40 ℃ in n-hexane, the esterification rate reached 96.6% after 10 h, and the esterification rate was still above 85.0% after six recycles.

    Solvothermal synthesis of N-doped TiO2 nanoparticles using different nitrogen sources, and their photocatalytic activity for degradation of benzene
    Fei He, Fang Ma, Tao Li, Guangxing Li
    2013, 34 (12):  2263-2270.  DOI: 10.1016/S1872-2067(12)60722-0
    Abstract ( 477 )   [Full Text(HTML)] () PDF (800KB) ( 952 )  

    Anatase-brookite mixed-phase N-doped TiO2 (N-TiO2) nanoparticles were synthesized through a solvothermal method using different nitrogen sources. The resulting samples were characterized by X-ray diffraction, specific surface area measurement, X-ray photoelectron spectroscopy, and standard and high-resolution transmission electron microscopy. The effects of the different nitrogen sources on phase composition, particle size, microstructure, and specific surface area are investigated. The photocatalytic activity of the TiO2 samples was evaluated through photocatalytic degradation of gaseous benzene under UV-light irradiation. N-TiO2 prepared using hydrazine hydrate achieved the highest photocatalytic performance in all the samples studied (including the commercial P25). Different intermediates during the photocatalytic degradation of benzene over HNT were identified by GC-MS analysis. A detailed reaction mechanism was proposed to explain their formation as intermediates in the reaction. Moreover, the photocatalytic activity of the nanoparticles remained almost unchanged after 15 gaseous-benzene degradation test cycles.

    Alumina-carbon nanotube supports for sulfur-resistant regenerable Pt-based catalysts in NOx reduction
    Lilong Jiang, Yuling Wang, Xian Liu, Yanning Cao, Kemei Wei
    2013, 34 (12):  2271-2276.  DOI: 10.1016/S1872-2067(12)60745-1
    Abstract ( 280 )   [Full Text(HTML)] () PDF (719KB) ( 616 )  

    Alumina-carbon nanotube (Al2O3-CNT) supports were prepared by the decomposition of acetylene on Al2O3. The subsequent impregnation of Pt and Ba yielded Pt/Ba/Al2O3-CNT. Pt/Ba/Al2O3-CNT was characterized by X-ray diffraction, scanning and transmission electron microscopies, N2 physisorption, X-ray photoelectron spectroscopy, and in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The relationship between the structure and properties of Pt/Ba/Al2O3-CNT was investigated. Pt/Ba/Al2O3-CNT exhibited much higher resistance to SO2 poisoning and better regeneration ability than Pt/Ba/Al2O3, during NOx reduction in the presence of SO2. In-situ DRIFTS spectra suggested that SO2 had no effect on the NOx storage and reduction process.