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    Chinese Journal of Catalysis
    2014, Vol. 35, No. 11
    Online: 06 November 2014

    Cover:

    Zheng and coworkers in their Article on pages 1800–1810 investigated the structure-directing behavior of different seeds in the organic structure- directing agent-free synthesis of zeolite Beta. The dissolution of seeds and the appearance of relatively scattered small crystals in microsized seed-directed synthesis indicated that the secondly nucleation was induced by the fragments from dissolved seeds.

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    Table of Contents
    Table of Contents for VOL.35 No.11
    2014, 35 (11):  0-0. 
    Abstract ( 167 )   PDF (1503KB) ( 575 )  
    Review
    Recent developments in photocatalytic dye degradation upon irradiation with energy-efficient light emitting diodes
    Wan-Kuen Jo, Rajesh J. Tayade
    2014, 35 (11):  1781-1792.  DOI: 10.1016/S1872-2067(14)60205-9
    Abstract ( 332 )   [Full Text(HTML)] () PDF (608KB) ( 1646 )  

    Light emitting diodes (LEDs) are gaining recognition as a convenient and energy-efficient light source for photocatalytic application. This review focuses on recent progress in the research and development of the degradation of dyes in water under LED light irradiation and provides a brief overview of photocatalysis, details of the LEDs commonly employed, a discussion of the advantages of LEDs over traditional ultraviolet sources and their application to photocatalytic dye degradation. We also discuss the experimental conditions used, the reported mechanisms of dye degradation and the various photocatalytic reactor designs and pay attention to the different types of LEDs used, and their power consumption. Based on a literature survey, the feasibility, benefits, limitations, and future prospects of LEDs for use in photocatalytic dye degradation are discussed in detail.

    Communication
    PVP-NiB amorphous catalyst for selective hydrogenation of phenol and its derivatives
    Qinsheng Zhang, Haifeng Li, Ping Gao, Lailai Wang
    2014, 35 (11):  1793-1799.  DOI: 10.1016/S1872-2067(14)60203-5
    Abstract ( 332 )   [Full Text(HTML)] () PDF (652KB) ( 856 )  

    PVP-NiB amorphous catalysts were prepared by the chemical reduction of nickel chloride with sodium borohydride, and characterized by infrared, X-ray diffraction, transmission election microscopy, and inductively coupled plasma. The relationship between the catalytic activity and nature of the active sites was discussed. PVP is a protective agent for preparing PVP-stabilized NiB catalysts, which improved the dispersion of the catalyst and stabilized its amorphous structure. The catalysis of phenol and its derivatives was evaluated in the aqueous phase. 99.9% conversion of phenol and 99.9% selectivity to cyclohexanol were obtained at 30 ℃ and 0.2 MPa H2 after 18 h over PVP-NiB. The generality of the PVP-NiB catalyst for this reaction was demonstrated by the selective hydrogenation of other phenol derivatives, which showed that the PVP-NiB catalyst was selective for the formation of cyclohexanol.

    Articles
    Mechanism of seeding in hydrothermal synthesis of zeolite Beta with organic structure-directing agent-free gel
    Bumei Zheng, Yufeng Wan, Weiya Yang, Fengxiang Ling, Hong Xie, Xiangchen Fang, Hongchen Guo
    2014, 35 (11):  1800-1810.  DOI: 10.1016/S1872-2067(14)60089-9
    Abstract ( 316 )   [Full Text(HTML)] () PDF (3175KB) ( 1168 )  

    The organic structure-directing agent-free synthesis of zeolite Beta was carried out using several zeolite Beta seeds that differed in SiO2/Al2O3 ratio and crystal size. The synthesis was studied using X-ray diffraction, X-ray fluorescence, scanning electron microscopy, transmission electron microscopy, ultraviolet-Raman spectroscopy, infrared spectroscopy, and N2 physisorption. Synthesis was successful using different zeolite Beta seeds including pure silica seeds. During the induction period, the seeds underwent dissolution. The SiO2/Al2O3 ratio and crystal size, pretreatment (calcination), and seed addition time had a significant influence on seed dissolution behavior, crystallization process, and product. Morphological studies revealed that the seed residues produced by dissolution (except for pure silica) resulted in the formation of "immobilized" surface nuclei, which allowed for the dense growth of fresh small zeolite Beta crystals. The dissolved small seed fragments yielded dispersed nuclei, which formed relatively scattered small zeolite Beta crystals thought to be the main nuclei source of the pure silica seed. It is suggested that the use of an appropriately high SiO2/Al2O3 ratio, small size, and precalcined zeolite Beta seed is helpful for the synthesis of highly crystalline and pure zeolite Beta from the organic structure-directing agent-free gel.

    Comparison of cellobiose and glucose transformation to ethylene glycol
    Junying Zhang, Xiaofeng Yang, Baolin Hou, Aiqin Wang, Zhenlei Li, Hua Wang, Tao Zhang
    2014, 35 (11):  1811-1817.  DOI: 10.1016/S1872-2067(14)60151-0
    Abstract ( 456 )   [Full Text(HTML)] () PDF (510KB) ( 781 )  

    Cellobiose was used as a model feedstock to probe the reaction pathways of cellulose to ethylene glycol (EG). Its reactivity was compared with that of glucose using a catalyst composed of H2WO4 and Ru/C. EG can be produced by both the direct retro-aldol condensation of cellobiose and the retro-aldol condensation of glucose derived from cellobiose hydrolysis. The direct retro-aldol condensation of cellobiose further promoted the hydrolysis of cellobiose. Cellobiose has a lower reactivity for retro-aldol condensation than glucose, which decreased the formation rate of glycolaldehyde and made it more matched with the subsequent hydrogenation rate, thus leading to increased yield of EG from cellobiose.

    Recyclable hydrophobic copper (Ⅱ) phthalocyanine catalyzed N-arylation of imidazoles in dimethylsulfoxide
    Qiang Huang, Limei Zhou, Xiaohui Jiang, Xiaolong Qi, Zhonghua Wang, Wencheng Lang
    2014, 35 (11):  1818-1824.  DOI: 10.1016/S1872-2067(14)60148-0
    Abstract ( 279 )   [Full Text(HTML)] () PDF (601KB) ( 553 )  

    Copper (Ⅱ) phthalocyanine (CuPc) was used as a catalyst for the N-arylation of imidazoles with aryl iodides or bromides. The catalyst showed high activity and could be reused 3 times without any significant loss in activity. The catalyst was characterized by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and ultraviolet-visible spectroscopy.

    Rhodamine B degradation and reactive oxygen species generation by a ZnSe-graphene/TiO2 sonocatalyst
    Lei Zhu, Sun-Bok Jo, Shu Ye, Kefayat Ullah, Won-Chun Oh
    2014, 35 (11):  1825-1832.  DOI: 10.1016/S1872-2067(14)60158-3
    Abstract ( 214 )   [Full Text(HTML)] () PDF (1877KB) ( 749 )  

    Nanostructured ZnSe-graphene/TiO2 was synthesized by a hydrothermal-assisted approach. ZnSe-graphene/TiO2 exhibited favorable adsorption of rhodamine B, a wide wavelength absorption range, and efficient charge separation. Reactive oxygen species were generated by the oxidation of 1,5-diphenyl carbazide to 1,5-diphenyl carbazone. The sonocatalytic reaction mechanism was proposed. These findings potentially broaden the applications of sonocatalytic technologies.

    Hydrogen production from decalin dehydrogenation over Pt-Ni/C bimetallic catalysts
    Suitao Qi, Yingying Li, Jiaqi Yue, Hao Chen, Chunhai Yi, Bolun Yang
    2014, 35 (11):  1833-1839.  DOI: 10.1016/S1872-2067(14)60178-9
    Abstract ( 298 )   [Full Text(HTML)] () PDF (582KB) ( 761 )  

    Pt-Ni bimetallic catalysts and the corresponding monometallic Pt catalysts supported on active carbon were prepared by incipient wetness impregnation and characterized by X-ray diffraction, N2 adsorption, and NH3-temperature programmed desorption. Their activities for decalin dehydrogenation were investigated at a superheated liquid film state in a batch reactor. The effects of temperature, impregnation sequence, and Pt/Ni molar ratio on the dehydrogenation activity and the naphthalene yield were investigated. The results show that the Pt-Ni bimetallic catalyst significantly enhanced hydrogen evolution compared with either Ni or Pt monometallic catalyst. The highest dehydrogenation conversion and naphthalene yield were obtained when the Pt/Ni molar ratio was 1:1 and Pt was impregnated first. The experimental results were correlated with density functional theory calculations of hydrogen binding energy (HBE) on different catalytic surfaces. The correlation confirmed that bimetallic surfaces with stronger HBEs had higher dehydrogenation activities.

    Rh(Ⅲ)-catalyzed synthesis of (dihydro)quinolines via the annulation of N-sulfonyl 2-aminobenzaldehydes with olefins
    Yimeng Zhang, Tao Zhang, Haoqiang Zhan, Xingwei Li
    2014, 35 (11):  1840-1845.  DOI: 10.1016/S1872-2067(14)60160-1
    Abstract ( 402 )   [Full Text(HTML)] () PDF (504KB) ( 756 )  

    We developed a new synthetic method for the production of 1,2-dihydroquinolines and quinolines via the Rh(Ⅲ)-catalyzed annulation of N-sulfonyl 2-aminobenzaldehydes with olefins. Various functionalities were found to be compatible under the operationally simple conditions. This study provides the first example of a Rh(Ⅲ)-catalyzed synthesis of 1,2-dihydroquinolines.

    Synergistic effect on Au-Pd bimetallic catalyst during oxidation of benzyl alcohol to sodium benzoate
    Zhaoyan Zhang, Ying Wang, Xian Li, Wei-Lin Dai
    2014, 35 (11):  1846-1857.  DOI: 10.1016/S1872-2067(14)60159-5
    Abstract ( 399 )   [Full Text(HTML)] () PDF (2435KB) ( 1012 )  

    A series of AuPd/CeO2 bimetallic catalysts with different Au/Pd molar ratios were investigated and their catalytic performance in the oxidation of benzyl alcohol to sodium benzoate and benzoic acid under solvent-free conditions was studied. The supported catalysts were characterized by X-ray diffraction, UV-Vis diffuse reflectance spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. The Au-Pd nanoparticles were successfully deposited onto CeO2 as a homogeneous alloy. The activity of the bimetallic catalysts was superior to that of the corresponding monometallic catalysts. This improvement was attributed to the synergistic effect between Au and Pd. The catalyst with an Au/Pd molar ratio of 3/1 showed the best catalytic performance (the yield of benzoic acid reached 92%), and it could be easily recovered and reused for more than seven successive reactions without significant loss of activity.

    Synthesis of benzo[g]indeno[2,1-b]quinoline derivatives via four-component and one-pot synthesis in presence of 3-methyl-1-sulfonic acid imidazolium hydrogen sulfate
    Nader Ghaffari Khaligh
    2014, 35 (11):  1858-1863.  DOI: 10.1016/S1872-2067(14)60186-8
    Abstract ( 217 )   [Full Text(HTML)] () PDF (367KB) ( 691 )  

    A simple and facile synthesis of 12-arylbenzo[g]indeno[2,1-b]quinoline-6,11,13-trione derivatives was accomplished by the one-pot condensation of 2-hydroxynaphthalene-1,4-dione, aryl aldehydes, 2H-indene-1,3-dione, and ammonium acetate under solvent-free conditions in the presence of a Brönsted ionic liquid catalyst, namely 3-methyl-1-sulfonic acid imidazolium hydrogen sulfate.

    CuI/N4 ligand/TEMPO derivatives: A mild and highly efficient system for aerobic oxidation of primary alcohols
    Shufang Zhang, Chengxia Miao, Daqian Xu, Wei Sun, Chungu Xia
    2014, 35 (11):  1864-1873.  DOI: 10.1016/S1872-2067(14)60161-3
    Abstract ( 237 )   [Full Text(HTML)] () PDF (753KB) ( 609 )  

    A new system consisting of a copper(I) complex generated in situ from a tetradentate nitrogen ligand and CuI in combination with 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) derivatives was successfully developed. The system was suitable for efficient and selective aerobic oxidation of primary benzyl and allyl alcohols with a wide range of functional groups to the corresponding aldehydes at room temperature. The best result was obtained with N,N'-dimethyl-N,N'-bis(2- pyridylmethyl)ethane-1,2-diamine as the ligand and 4-OH-TEMPO as a cocatalyst in CH3CN. In addition, high-resolution mass spectrometry, ultraviolet-visible spectroscopy, and electrochemical experiments were used to provide evidence of intermediates.

    Preparation and catalytic performance of perfluorosulfonic acid-functionalized carbon nanotubes
    Mengxiao Zhang, Cuican Li, Weiming Hua, Yinghong Yue, Zi Gao
    2014, 35 (11):  1874-1882.  DOI: 10.1016/S1872-2067(14)60167-4
    Abstract ( 268 )   [Full Text(HTML)] () PDF (959KB) ( 571 )  

    Perfluorosulfonic acid-functionalized carbon nanotubes were prepared by liquid deposition of the perfluorosulfonic acid-polytetrafluoroethylene copolymer and characterized by N2 adsorption, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, and acid-base titration. The effects of reaction temperature and the type of solvent were investigated. The results showed that these solid acids are very stable in both polar and non-polar solvents and can maintain their acidity up to 300 ℃. Higher activity and better stability were observed over these materials in the alkylation of hydroquinone compared with poly(styrene sulfonic acid)-grafted carbon nanotubes.

    Effect of preparation method on the performance of Pd-MnOx/γ-Al2O3 monolithic catalysts for ground-level O3 decomposition
    Chengjun Ren, Lina Zhou, Hongyan Shang, Yaoqiang Chen
    2014, 35 (11):  1883-1891.  DOI: 10.1016/S1872-2067(14)60176-5
    Abstract ( 228 )   [Full Text(HTML)] () PDF (588KB) ( 699 )  

    MnOx +γ-Al2O3 and MnOx/γ-Al2O3 catalysts were prepared by the sol-gel and sequential precipitation methods, respectively. The same amount of Pd was loaded on these catalysts by incipient wetness impregnation. The two Pd-MnOx/γ-Al2O3 catalysts with different physicochemical properties were coated on cordierite. The catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, and N2 adsorption-desorption measurement. The preparation method and calcination temperature of MnOx have significant impact on the crystalline phase of MnOx, MnOx species and active oxygen species, and textural properties of the catalysts. The experimental results showed that 0.60 μL·L-1 of ozone was completely decomposed on these catalysts in the temperature range of 16 to 90 ℃ at space velocities from 380000 to 580000 h-1. In particular, the activity for O3 decomposition was excellent on the Pd/MnOx+Pd/γ-Al2O3 catalyst that used MnOx prepared by the sol-gel method. Mnn+ is beneficial for O3 decomposition, and Mn2+, Mn3+, and Mn4+ were presented in a mole ratio of 1.7:1:3 on the surface of the catalyst.

    Hierarchical ZSM-5 catalyst synthesized by a Triton X-100 assisted hydrothermal method
    S. Narayanan, J. Judith Vijaya, S. Sivasanker, Sihai Yang, L. John Kennedy
    2014, 35 (11):  1892-1989.  DOI: 10.1016/S1872-2067(14)60177-7
    Abstract ( 242 )   [Full Text(HTML)] () PDF (1111KB) ( 759 )  

    ZSM-5 zeolite with a hexagonal cubic morphology was synthesized by a hydrothermal method using Triton X-100, a nonionic surfactant. The samples prepared with and without the surfactant were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy, N2 adsorption, high resolution transmission electron microscopy (TEM), high resolution scanning electron microscopy, energy dispersive X-ray analysis, and NH3 temperature-programmed desorption. The XRD patterns confirmed the formation of a pure ZSM-5 crystalline phase without secondary phases. TEM images revealed that the hexagonal cubes were made of peanut-shaped nanoparticles with voids. The catalytic activity of the zeolite samples was evaluated using the selective oxidation of benzyl alcohol with tertiary-butyl hydrogen peroxide as the oxidant at 90 ℃. The surfactant-assisted preparation yielded a zeolite that gave a higher conversion than the one prepared in the absence of the surfactant. The catalyst was retrieved and reused four times without significant loss in activity and selectivity.

    Effect of Pt cocatalyst in Pt/TiO2 studied by in situ FTIR of CO adsorption
    Shuai Shen, Xiuli Wang, Qian Ding, Shaoqing Jin, Zhaochi Feng, Can Li
    2014, 35 (11):  1990-1906.  DOI: 10.1016/S1872-2067(14)60172-8
    Abstract ( 417 )   [Full Text(HTML)] () PDF (780KB) ( 935 )  

    In situ transmission infrared spectroscopy was used to study the role of Pt cocatalyst in Pt/TiO2 using CO as a probe molecule. An 11 cm-1 redshift of CO adsorbed on Pt/TiO2 was observed under irradiation in the absence of changes in the CO coverage or sample temperature. In contrast, no CO shift was detected on Pt/Al2O3. This indicates that the redshift of the CO adsorption peak is due to the photogenerated electron transfer from TiO2 to Pt, and this accounts for the increased photocatalytic activity by the loaded Pt cocatalyst.