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? 催化学报
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Chinese Journal of Catalysis
2017, Vol.38 No.3
Online: 18 March 2017


Contents | Special Column on New Porous Catalytic Materials | Articles |

Catalysis is the key to creating new energy and to protecting environments for the sustainable development of the world as discussed in ICC 2016 in Beijing.For this purpose,we need to reinforce catalytic science and technology and to extend our findings to innovation.This special column invited four papers on biomass conversion and transformation of CO2,which contributes to the progress of heterogeneous catalysis.

 
Contents
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Table of Contents for VOL.38 No.3
2017 Vol. 38 (3): 0-0 [Abstract] ( 8 ) [Full Text(HTML)] () 1KB] [PDF 0KB] ( 1 )    DOI:

Special Column on New Porous Catalytic Materials
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Professor Atsushi Fukuoka
Preface to Special Column on Novel Catalysts for Energy and Environmental Issues
2017 Vol. 38 (3): 419-419 [Abstract] ( 8 ) [Full Text(HTML)] () 1KB] [PDF 213KB] ( 11 )    DOI: 10.1016/S1872-2067(17)62803-1

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Hirokazu Kobayashi, Shogo Ito, Kenji Hara, Atsushi Fukuoka
Conversion of glycerol to acrolein by mesoporous sulfated zirconia-silica catalyst
2017 Vol. 38 (3): 420-425 [Abstract] ( 11 ) [Full Text(HTML)] () 1KB] [PDF 628KB] ( 25 )    DOI: 10.1016/S1872-2067(16)62564-0

A mesoporous sulfated zirconia-silica catalyst bearing only Brønsted acid sites converted glycerol to acrolein in 81% yield with 82% selectivity. Space time yield as high as 9.0 mmol h-1 gcat-1 was achieved even at a low reaction temperature of 523 K. The catalytic activity and selectivity were higher than those of typical sulfated zirconia. It is proposed that the milder acidity due to dilution of zirconium species by silica and large pore size for faster diffusion contributed towards the better catalytic performance.

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Asep Bayu, Surachai Karnjanakom, Katsuki Kusakabe, Abuliti Abudula, Guoqing Guan
Preparation of Sn-β-zeolite via immobilization of Sn/choline chloride complex for glucose-fructose isomerization reaction
2017 Vol. 38 (3): 426-433 [Abstract] ( 13 ) [Full Text(HTML)] () 1KB] [PDF 1357KB] ( 30 )    DOI: 10.1016/S1872-2067(17)62754-2

Well dispersion of tin species in an isolated form is a quite challenge since tin salts are easily hydrolyzed into (hydr)oxides during aqueous stannation of β-zeolite. In this study, immobilization of tin species on high silica commercial β-zeolite by using SnCl2/Choline chloride (ChCl) complex followed with calcination provided a convenient way to get well dispersed Sn in β-zeolite in the aqueous condition, which was observed based on electron microscopy images, UV visible spectra and X-ray diffraction pattern. The existence of ChCl facilitated tin species to incorporate into zeolite. (1-2) wt% of Sn loaded β-zeolites exhibited good catalytic activity and high selectivity for glucose-fructose isomerization reaction.

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Ken Motokura, Masaki Naijo, Sho Yamaguchi, Akimitsu Miyaji, Toshihide Baba
Reductive transformation of CO2: Fluoride-catalyzed reactions with waste silicon-based reducing agents
2017 Vol. 38 (3): 434-439 [Abstract] ( 6 ) [Full Text(HTML)] () 1KB] [PDF 834KB] ( 22 )    DOI: 10.1016/S1872-2067(17)62800-6

CO2 is one of the most important “renewable” carbon sources. To transform CO2 to useful organic compounds, we examined the reactivity of two model silicon-based “waste” materials, disilanes and metallic Si powder, as reducing agents. In these reactions, fluoride salts were found to be active catalysts: CO2 was converted to formic acid at atmospheric pressure in the presence of H2O as a proton source and the silicon-based reducing reagents. Based on in-situ NMR and kinetics analyses, a hydrosilane and penta-coordinate Si species are proposed as the reaction intermediate and active species, respectively.

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Bo Yuan, Bao Zhang, Zhiliang Wang, Shengmei Lu, Jun Li, Yan Liu, Can Li
Photocatalytic aerobic oxidation of toluene and its derivatives to aldehydes on Pd/Bi2WO6
2017 Vol. 38 (3): 440-446 [Abstract] ( 12 ) [Full Text(HTML)] () 1KB] [PDF 854KB] ( 20 )    DOI: 10.1016/S1872-2067(17)62757-8

The selective oxidation of toluene and its derivatives is extremely important in the chemical industry.The use of photocatalysis in organic synthesis has attracted considerable attention among synthetic chemists because of its “green” environmental characteristics. In this study, nanoscale Bi2WO6 with a flower-like morphology was found to be a highly efficient photocatalyst in the catalytic oxidation of toluene and its derivatives using O2 as the oxidant. The loading of Pd nanoparticles as a cocatalyst onto the flower-like Bi2WO6 was found to produce a significant enhancement in the catalytic activity. Mechanistic investigation showed that the superior performance of Pd/Bi2WO6 could be attributed to the improvement of both the reductive and oxidative abilities of Bi2WO6 by the loading of the cocatalyst.

Articles
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Xu Tang, Liang Ni, Juan Han, Yun Wang
Preparation and characterization of ternary magnetic g-C3N4 composite photocatalysts for removal of tetracycline under visible light
2017 Vol. 38 (3): 447-457 [Abstract] ( 7 ) [Full Text(HTML)] () 1KB] [PDF 1060KB] ( 16 )    DOI: 10.1016/S1872-2067(16)62591-3

A stable PNIPAM/Fe3O4/g-C3N4 composite photocatalyst was designed and prepared by a thermal photoinitiation technology. The structure and properties of the materials were characterized and the composite photocatalyst was found to show good stability for tetracycline degradation. The sample not only retained the magnetic properties of Fe3O4, allowing it to be recycled, but its photocatalytic properties could also be changed by controlling the temperature of the reaction system. The degradation intermediate products of tetracycline were further investigated by MS. This work provides a new facile strategy for the development of intelligent and recyclable photocatalytic materials.

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Ezzat Rafiee, Maryam Khodayari
Synthesis and characterization of PMoV/Fe3O4/g-C3N4 from melamine: An industrial green nanocatalyst for deep oxidative desulfurization
2017 Vol. 38 (3): 458-468 [Abstract] ( 3 ) [Full Text(HTML)] () 1KB] [PDF 1301KB] ( 13 )    DOI: 10.1016/S1872-2067(16)62548-2

A facile approach to the preparation of a novel magnetically separable H5PMo10V2O40/Fe3O4/g-C3N4 (PMoV/Fe3O4/g-C3N4) nanocomposite by chemical impregnation is demonstrated. The prepared nanocomposite was characterized and its acidity was measured by potentiometric titration. PMoV/Fe3O4/g-C3N4 showed high catalytic activity in the selective oxidative desulfurization of sulfides to their corresponding sulfoxides or sulfones. The catalytic oxidation of a dibenzothiophene (DBT)-containing model oil and that of real oil were also studied under optimized conditions. In addition, the effects of various nitrogen compounds, as well as the use of one- and two-ring aromatic hydrocarbons as co-solvents, on the catalytic removal of sulfur from DBT were investigated. The catalyst was easily separated and could be recovered from the reaction mixture by using an external magnetic field. Additionally, the remaining reactants could be separated from the products by simple decantation if an appropriate solvent was chosen for the extraction. The advantages of this nanocatalyst are its high catalytic activity and reusability; it can be used at least four times without considerable loss of activity.

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Arash Ghorbani-Choghamarani, Zahra Taherinia
Synthesis of biaryls using palladium nanoparticles immobilized on peptide nanofibers as catalyst and hydroxybenzotriazole as novel phenylating reagent
2017 Vol. 38 (3): 469-474 [Abstract] ( 6 ) [Full Text(HTML)] () 1KB] [PDF 1861KB] ( 19 )    DOI: 10.1016/S1872-2067(17)62586-X

Peptide nanofibers decorated with palladium nanoparticles catalyzed direct coupling of aryl halides with hydroxybenzotriazole to afford the corresponding biaryls in good to excellent yields. The coupling reactions proceeded under simple, green, and mild conditions. The peptide nanofibers were used as recyclable supports in the coupling reactions. This approach is the first to use hydroxybenzotriazole as a phenylating agent.

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Shirish S. Punde, Bruce J. Tatarchuk
Pt-CeO2/SiO2 catalyst for CO oxidation in humid air at ambient temperature
2017 Vol. 38 (3): 475-488 [Abstract] ( 7 ) [Full Text(HTML)] () 1KB] [PDF 4613KB] ( 18 )    DOI: 10.1016/S1872-2067(17)62749-9

CO self-poisoning and slow surface kinetics pose major challenges to a CO oxidation catalyst that should work at ambient temperature. Furthermore, the presence of moisture would cause passivation of the catalyst. A highly active ceria promoted Pt catalyst (4%Pt-12%CeO2/SiO2; conversion ≥ 99% at low (< 500 ppm) and high (> 2500 ppm) CO concentrations was developed for CO oxidation at ambient temperature in humid air. Catalyst preparation variables such as Pt and CeO2 loading, ceria deposition method, drying and calcination conditions for the ceria and Pt precursors were optimized experimentally. The activity was correlated with surface properties using CO/H2 chemisorption, O2-H2 titration, X-ray diffraction and BET surface area analysis. The method of CeO2 deposition had a significant impact on the catalytic activity. CeO2 deposition by impregnation resulted in a catalyst that was three times more active than that prepared by deposition precipitation or CeO2 grafting. O2-H2 titration results revealed that the close association of ceria and Pt in the case of CeO2 deposition by impregnation resulted in higher activity. The catalyst support used was also crucial as a silica supported catalyst was five times more active than an alumina supported catalyst. The particle size and pore structure of the catalyst support were also crucial as the reaction was diffusion controlled. The drying and calcination conditions of the ceria and Pt precursors also played a crucial role in determining the catalytic activity. The Pt-CeO2/SiO2 catalysts with Pt > 2.5 wt% and CeO2 > 15 wt% were highly active (TOF > 0.02 s-1) and stable (conversion ≥ 99% after 15 h) at ambient conditions.

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Jinzhan Su, Tao Zhang, Lu Wang, Jinwen Shi, Yubin Chen
Surface treatment effect on the photocatalytic hydrogen generation of CdS/ZnS core-shell microstructures
2017 Vol. 38 (3): 489-497 [Abstract] ( 4 ) [Full Text(HTML)] () 1KB] [PDF 1612KB] ( 15 )    DOI: 10.1016/S1872-2067(17)62769-4

CdS/ZnS core-shell microparticles were prepared by a simple two-step method combining ultrasonic spray pyrolysis and chemical bath deposition. The core-shell structures showed enhanced photocatalytic properties compared with those of CdS or ZnS spherical particles. CdS/ZnS photocatalysts with different amount of ZnS loaded as shells were prepared by adjusting the concentrations of Zn and S precursors during synthesis. The optical properties and photocatalytic activity for hydrogen production were investigated and the amount of ZnS loaded as shell was optimized. Thermal annealing and hydrothermal sulfurization treatments were applied to the core-shell structure and both treatments enhanced the material's photocatalytic activity and stability by eliminating crystalline defects and surface states. The result showed that thermal annealing treatment improved the bulk crystallinity and hydrothermal sulfurization improved the surface properties. The sample subjected to both treatments showed the highest photocatalytic activity. These results indicate that CdS/ZnS core-shell microspheres are a simple structure that can be used as efficient photocatalysts. The hydrothermal sulfurization treatment may also be a useful surface treatment for metal sulfide photocatalysts. The simple two-step method provides a promising approach to the large-scale synthesis of core-shell microsphere catalysts.

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Zhenxing Zeng, Kexin Li, Kai Wei, Yuhua Dai, Liushui Yan, Huiqin Guo, Xubiao Luo
Fabrication of porous g-C3N4 and supported porous g-C3N4 by a simple precursor pretreatment strategy and their efficient visible-light photocatalytic activity
2017 Vol. 38 (3): 498-508 [Abstract] ( 4 ) [Full Text(HTML)] () 1KB] [PDF 913KB] ( 22 )    DOI: 10.1016/S1872-2067(17)62763-3

Porous g-C3N4 and supported porous g-C3N4 were fabricated for the first time by a simple strategy using pretreated melamine as a raw material and pretreated quartz rod as a substrate. The formation of a richly porous microstructure can be attributed to the co-existence of different pore-fabricating units in the preparation system for porous g-C3N4. The richly porous microstructure endowed the as-prepared porous g-C3N4 with an excellent photocatalytic activity. The as-prepared supported porous g-C3N4 exhibited considerable stability because of the existence of chemical interaction between porous g-C3N4 and the quartz rod substrate. The photocatalytic activity of the supported porous g-C3N4 was competitive with that of porous g-C3N4 in powder form because neither the surface migration of photogenerated electrons nor the diffusion of the target organic pollutant were affected by the construction of the quartz rod reactor. The photocatalytic activity of the as-prepared porous g-C3N4 and supported porous g-C3N4 was preliminarily evaluated by the treatment of single-component organic wastewater under visible-light irradiation. Subsequently, the as-prepared porous g-C3N4 was further applied in conventional hydrogen evolution and a new system for simultaneous hydrogen evolution with organic-pollutant degradation. The hydrogen yield and degradation efficiency both increased with increasing photocatalytic activity of the as-prepared materials in the system for simultaneous hydrogen evolution with organic-pollutant degradation.

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Zhichao Yang, Yunqi Liu, Jinchong Zhao, Jianxia Gou, Kaian Sun, Chenguang Liu
Zinc-modified Pt/SAPO-11 for improving the isomerization selectivity to dibranched alkanes
2017 Vol. 38 (3): 509-517 [Abstract] ( 8 ) [Full Text(HTML)] () 1KB] [PDF 2556KB] ( 31 )    DOI: 10.1016/S1872-2067(17)62755-4

Zinc-modified Pt/SAPO-11 catalysts were prepared by incipient wetness impregnation and assessed in the hydroisomerization of n-octane. Their physicochemical properties were investigated using powder X-ray diffraction, scanning electron microscopy, nitrogen adsorption-desorption, pyridine-adsorbed infrared spectroscopy, temperature-programmed desorption of NH3, temperature-programmed reduction of hydrogen, temperature-programmed desorption of hydrogen, transmission electron microscopy, and X-ray photoelectron spectroscopy. The addition of zinc resulted in high dispersion of platinum. Zinc acted as a competitive adsorbent, changed the location of platinum. The catalyst with a zinc loading of 0.5% gave the highest selectivity to dimethylhexanes, but the conversion was lower than those achieved with the other catalysts. Dimethylhexanes have large molecular diameters, and therefore their diffusion may be difficult. This weakens the catalytic activity of the zinc-modified catalysts and lowers the n-octane conversion.

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Baitao Li, Xin Luo, Jing Huang, Xiujun Wang, Zhenxing Liang
One-pot synthesis of ordered mesoporous Cu-KIT-6 and its improved catalytic behavior for the epoxidation of styrene: Effects of the pH value of the initial gel
2017 Vol. 38 (3): 518-528 [Abstract] ( 5 ) [Full Text(HTML)] () 1KB] [PDF 2334KB] ( 10 )    DOI: 10.1016/S1872-2067(17)62767-0

The heterogeneously copper-catalyzed oxidative cleavage of styrene was studied using copper-doped mesoporous KIT-6 (Cu-KIT-6x) prepared via pH adjustment (where x is the pH: 1.43, 2.27, 3.78, 3.97, 4.24 or 6.62). Variations in the catalyst structure and morphology with pH values were characterized by X-ray power diffraction, nitrogen adsorption-desorption analysis, transmission electron microscopy and X-ray photoelectron spectroscopy. As the pH value applied during the initial synthesis, the resulting Cu-KIT-6x exhibited different structural, textural and surface characteristics, especially in terms of specific copper species and copper content. At a pH value of 3.78, approximately 4.6 wt% copper(II) was successfully incorporated into the framework of the initial KIT-6, in the form of -Cu-O-Si- groups. The catalytic performance of each catalyst was evaluated by following the epoxidation of styrene, employing tert-butyl hydroperoxide as the oxidant and CH3CN as the solvent. A significant styrene conversion of 43.5% with 86.6% selectivity for the desired styrene epoxide was obtained over the Cu-KIT-63.78. A higher Cu content, an ordered cubic Ia3d mesoporous architecture and various specific textural characteristics all combined to endow the Cu-KIT-63.78 with high catalytic activity and good stability.

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Hualan Zhou, Jingjing Gong, Bolian Xu, Shengcai Deng, Yuanhua Ding, Lei Yu, Yining Fan
PtSnNa/SUZ-4: An efficient catalyst for propane dehydrogenation
2017 Vol. 38 (3): 529-536 [Abstract] ( 16 ) [Full Text(HTML)] () 1KB] [PDF 601KB] ( 13 )    DOI: 10.1016/S1872-2067(17)62750-5

The structure and catalytic properties of PtSn catalysts supported on SUZ-4 and ZSM-5 zeolite have been studied by using various experimental techniques including XRD, nitrogen adsorption, NH3-TPD, TG, H2-TPR and TPO techniques combined with propane dehydrogenation tests. It has been shown that SUZ-4-supported PtSnNa (PtSnNa/SUZ-4) was determined to be a better catalyst for propane dehydrogenation than conventional catalysts supported on ZSM-5, owing to its higher catalytic activity and stability. Dibenzothiophene poisoning experiments were performed to investigate the detailed structures of the two supported catalysts. The characterization of the two catalysts indicates that the distribution of Pt on the porous support affects the activity. In contrast to ZSM-5-supported catalysts, Pt particles on the PtSnNa/SUZ-4 are primarily dispersed over the external surface and are not as readily deactivated by carbon deposition. This is because that the strong acid sites of the SUZ-4 zeolite evidently prevented the impregnation of the Pt precursor H2PtCl6 into the zeolite. In contrast, the weak acid sites of the ZSM-5 zeolite led to more of the precursor entering the zeolite tunnels, followed by transformation to highly dispersed Pt clusters during calcination. In the case of the PtSnNa/ZSM-5, the interactions between Sn oxides and the support were lessened, owing to the weaker acidity of the ZSM-5 zeolite. The dispersed Sn oxides were therefore easier to reduce to the metallic state, thus decreasing the catalytic activity for hydrocarbon dehydrogenation.

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Mengyuan Zhang, Yanyan Sun, Juanjuan Shi, Wensheng Ning, Zhaoyin Hou
Selective glycerol oxidation using platinum nanoparticles supported on multi-walled carbon nanotubes and nitrogen-doped graphene hybrid
2017 Vol. 38 (3): 537-544 [Abstract] ( 25 ) [Full Text(HTML)] () 1KB] [PDF 1454KB] ( 25 )    DOI: 10.1016/S1872-2067(17)62761-X

Selective oxidation of glycerol is a hot topic. Increased biodiesel production has led to glycerol oxidation over Au- and Pt-based catalysts being widely studied. However, Pt catalysts suffer from deactivation because of weak metal-support interactions. In this study, multi-walled carbon nanotube (MWCNTs)-pillared nitrogen-doped graphene (NG) was prepared by direct pyrolysis of melamine on MWCNTs, and the synthesized NG-MWCNT composite was used as the support for Pt. Characterization results showed that the surface area (173 m2/g) and pore volume of the NG-MWCNT composite were greater than those of bare MWCNTs and the separated melamine pyrolysis product (CNx). Pt (1.4 ± 0.4 nm) dispersion on the NG-MWCNTs was favorable and the Pt/NG-MWCNT catalyst was highly active and selective in the oxidation of glycerol to glyceric acid (GLYA) in base-free aqueous solution. For example, the conversion of glycerol reached 64.4% with a GLYA selectivity of 81.0%, whereas the conversions of glycerol over Pt/MWCNTs and Pt/CNx were 29.0% and 31.6%, respectively. The unique catalytic activity of the Pt/NG-MWCNTs is attributed to well-dispersed Pt clusters on the NG-MWCNTs and the electron-donating effect of the nitrogen dopant in the NG-MWCNTs.

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Wei Hong, Xiaoqing Yan, Renhong Li, Jie Fan
Gold nanoparticle stabilization within tailored cubic mesoporous silica: Optimizing alcohol oxidation activity
2017 Vol. 38 (3): 545-553 [Abstract] ( 5 ) [Full Text(HTML)] () 1KB] [PDF 1971KB] ( 20 )    DOI: 10.1016/S1872-2067(17)62762-1

Stabilizing gold nanoparticles (AuNPs) within a desired size range is critical to realize their promising catalytic performance in many important reactions. Herein, we investigate the anti-sintering properties of cubic mesoporous silica (FDU-12) as a function of pore entrance size. Simple adjustments to the type of organic template and reaction temperature enable the successful synthesis of FDU-12 with controllable entrance sizes (< 3, 3-5 and 7 nm). Excellent anti-sintering properties are observed for FDU-12 with a sub-5-nm entrance size (3-5 nm) over a wide loading concentration (1.0-8.3 wt%) and the AuNPs can be stabilized within a 4.5-5.0-nm range after calcination at 550℃ in air for 5 h. Smaller entrance size (< 3 nm) prevents ingress of 3-nm AuNPs to the mesopores and results in low loading capacity and sintering. Conversely, FDU-12 possessing a larger entrance size (7 nm) shows promising anti-sintering properties at high loading concentrations, although catalytic performance is significantly lost at lower concentrations (e.g. 2.1 wt%, 14.2 ± 5.5 nm). Different anti-sintering mechanisms are proposed for each of the different FDU-12 entrance sizes. Additionally, catalytic data indicates that the obtained 4.5-nm AuNPs supported on FDU-12 with a sub-5-nm entrance size exhibit excellent mass-specific activity (1544 mmol gAu-1 h-1) and selectivity (> 99%) at 230℃ for the gas-phase selective oxidation of cyclohexanol.

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Guihua Song, Haifang Yang, Yafei Sun, Jingyi Wang, Weidong Qu, Qiang Zhang, Lingjuan Ma, Yuanyuan Feng
Promoting effects of Fe2O3 to Pt electrocatalysts toward methanol oxidation reaction in alkaline electrolyte
2017 Vol. 38 (3): 554-563 [Abstract] ( 1 ) [Full Text(HTML)] () 1KB] [PDF 895KB] ( 22 )    DOI: 10.1016/S1872-2067(17)62773-6

Fe2O3 nanorods and hexagonal nanoplates were synthesized and used as the promoters for Pt electrocatalysts toward the methanol oxidation reaction (MOR) in an alkaline electrolyte. The catalysts were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, cyclic voltammetry and chronoamperometry. The results show that the presence of Fe2O3 in the electrocatalysts can promote the kinetic processes of MOR on Pt, and this promoting effect is related to the morphology of the Fe2O3 promoter. The catalyst with Fe2O3 nanorods as the promoter (Pt-Fe2O3/C-R) exhibits much higher catalytic activity and stability than that with Fe2O3 nanoplates as the promoter (Pt-Fe2O3/C-P). The mass activity and specific activity of Pt in a Pt-Fe2O3/C-R catalyst are 5.32 A/mgPt and 162.7 A/mPt2, respectively, which are approximately 1.67 and 2.04 times those of the Pt-Fe2O3/C-P catalyst, and 4.19 and 6.16 times those of a commercial PtRu/C catalyst, respectively. Synergistic effects between Fe2O3 and Pt and the high content of Pt oxides in the catalysts are responsible for the improvement. These findings contribute not only to our understanding of the MOR mechanism but also to the development of advanced electrocatalysts with high catalytic properties for direct methanol fuel cells.

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Guchu Zou, Zeyun Fan, Xin Yao, Yi Zhang, Zhixiang Zhang, Mingxia Chen, Wenfeng Shangguan
Catalytic performance of Ag/Co-Ce composite oxides during soot combustion in O2 and NOx: Insights into the effects of silver
2017 Vol. 38 (3): 564-573 [Abstract] ( 7 ) [Full Text(HTML)] () 1KB] [PDF 584KB] ( 15 )    DOI: 10.1016/S1872-2067(17)62758-X

The composite oxides xAg/Co0.93Ce0.07 (x = Ag/(Co+Ce) molar ratio), intended for use as high performance catalytic materials, were successfully prepared via citric acid complexation. The effects of silver on the performance of these substances during soot combustion were subsequently investigated. Under O2, the 0.3Ag/Co0.93Ce0.07 catalyst resulted in the lowest ignition temperature, T10, of 197℃, while the minimum light-off temperature was obtained from both 0.2Ag/Co0.93Ce0.07 and 0.3Ag/Co0.93Ce0.07 in the NOx atmosphere. These materials were also characterized by various techniques, including H2, soot and NOx temperature programmed reduction, X-ray diffraction, and electron paramagnetic resonance, Raman, X-ray photoelectron, and Fourier transform infrared spectroscopic analyses. The results demonstrated that silver significantly alters the catalytic behavior under both O2 and NOx, even though the lattice structure of the mixed oxide is not affected. Surface silver oxides generated under the O2 atmosphere favor soot combustion by participating in the redox cycles between soot and the silver oxide, whereas the AgNO3 that forms in a NOx-rich atmosphere facilitates soot abatement at a lower temperature. The inferior activity of AgNO3 relative to that of Ag2O results in the different catalytic performance in the presence of NOx or O2.

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Yuyan Qiao, Pengfei Wu, Xiao Xiang, Miao Yang, Quanyi Wang, Peng Tian, Zhongmin Liu
SAPO-34 synthesized with n-butylamine as a template and its catalytic application in the methanol amination reaction
2017 Vol. 38 (3): 574-582 [Abstract] ( 3 ) [Full Text(HTML)] () 1KB] [PDF 1683KB] ( 25 )    DOI: 10.1016/S1872-2067(17)62775-X

SAPO-34 was synthesized with n-butylamine (BA) as a template for the first time. Crystallization temperature and initial Si amount were important factors leading to successful syntheses. Lamellar AlPO-kanemite tends to form as the major phase or as an impurity of SAPO-34 at lower crystallization temperatures, though a higher initial Si amount may offer a positive effect on the crystallization of SAPO-34 that mitigates the low temperature. Higher temperature (240℃) can effectively suppress the generation of lamellar materials and allow the synthesis of pure SAPO-34 with a wider range of Si incorporation. The crystallization processes at 200 and 240℃ were investigated and compared. We used the aminothermal method to synthesize SAPO-34-BA at 240℃ and also found n-propylamine is a suitable template for the synthesis of SAPO-34. The SAPO-34-BA products were characterized by many techniques. SAPO-34-BA has good thermal stability, crystallinity and porosity. BA remained intact in the crystals with ~1.8 BA molecule per chabazite cage. The catalytic performance of SAPO-34 was tested in the methanol amination reaction, which showed high methanol conversion and selectivity for methylamine plus dimethylamine under the conditions investigated, suggesting that this material is a good candidate for the synthesis of methylamines.

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Ling Zhang, Xue Liu, Rui-Xia Yang, Nian-Yu Huang, Wei-Qiao Deng
Environmentally benign and economic synthesis of covalent triazine-based frameworks
2017 Vol. 38 (3): 583-588 [Abstract] ( 4 ) [Full Text(HTML)] () 1KB] [PDF 683KB] ( 21 )    DOI: 10.1016/S1872-2067(17)62771-2

Covalent triazine-based frameworks (CTFs) are important microporous materials with a wide range of applications. Here, we demonstrate an environmentally benign and economic synthetic pathway to CTFs. The monomers used for CTFs, aromatic nitriles, were obtained by cyanation using nontoxic potassium hexacyanoferrate(II) in place of commonly used toxic cyanides. Then, the CTFs were synthesized by trimerization of the corresponding cyano monomers in molten zinc chloride. A series of CTFs was synthesized, and the highest Brunauer-Emmett-Teller surface area measured in this series was 2404 m2/g. Among the synthesized CTFs, CTFDCP exhibited excellent CO2 adsorption properties, with a CO2 uptake of 225 mg/g at 0℃.

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Haipeng Fan, Zhengliang Qi, Dejun Sui, Fei Mao, Rizhi Chen, Jun Huang
Palladium nanoparticles in cross-linked polyaniline as highly efficient catalysts for Suzuki-Miyaura reactions
2017 Vol. 38 (3): 589-596 [Abstract] ( 5 ) [Full Text(HTML)] () 1KB] [PDF 532KB] ( 17 )    DOI: 10.1016/S1872-2067(17)62772-4

Palladium nanoparticles supported on cross-linked polyaniline with bulky phosphorus ligands were developed. These catalysts showed high efficiency in the Suzuki-Miyaura reaction of aryl chlorides and bromides with phenylboronic acids. Aryl chlorides and bromides with functional groups, such as CN, MeO, CHO, MeCO and NO2, were converted to the corresponding biphenyls in high yields with catalyst loading. Additionally, the catalysts combined high activity with good reusability; they could be used at least five times for the Suzuki-Miyaura coupling reaction.

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Min Li, Donge Wang, Jiahe Li, Zhendong Pan, Huaijun Ma, Yuxia Jiang, Zhijian Tian, Anhui Lu
Surfactant-assisted hydrothermally synthesized MoS2 samples with controllable morphologies and structures for anthracene hydrogenation
2017 Vol. 38 (3): 597-606 [Abstract] ( 3 ) [Full Text(HTML)] () 1KB] [PDF 1835KB] ( 22 )    DOI: 10.1016/S1872-2067(17)62779-7

MoS2 samples with controllable morphologies and structures were synthesized using surfactant-assisted hydrothermal processes. The effects of surfactants (PEG, PVP, P123, SDS, AOT, and CTAB) on the morphologies and structures of MoS2 samples were investigated. The results revealed that spherical, bulk-like, and flower-like MoS2 particles assembled by NH4+-intercalated MoS2 nano-sheets were synthesized. The morphologies of the MoS2 samples and their structures (including the slab length and the number of stacked layers) of MoS2 nano-sheets in these samples could be controlled by adjusting the surfactants. Mono-dispersed spherical MoS2 particles could be synthesized with PEG via the creation of MoS2 nano-sheets with slab lengths shorter than 15 nm and fewer than six stacked layers. Possible formation mechanisms of these MoS2 samples created via surfactant-assisted hydrothermal processes are proposed. Further, the catalytic activities of MoS2 samples for anthracene hydrogenation were evaluated in a slurry-bed reactor. The catalyst synthesized with the surfactant PEG exhibited the highest catalytic hydrogenation activity. Compared with the other catalysts, it had a smaller particle size, mono-dispersed spherical morphology, shorter slab length, and fewer stacked layers; these were all beneficial to exposing its active edges. This work provides an efficient approach to synthesize transition metal sulfides with controllable morphologies and structures.

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Lei Gu, Xiao Chen, Ying Zhou, Qiulian Zhu, HaifengHuang, Hanfeng Lu
Propene and CO oxidation on Pt/Ce-Zr-SO42- diesel oxidation catalysts: Effect of sulfate on activity and stability
2017 Vol. 38 (3): 607-616 [Abstract] ( 2 ) [Full Text(HTML)] () 1KB] [PDF 588KB] ( 21 )    DOI: 10.1016/S1872-2067(17)62781-5

Platinum/cerium-zirconium-sulfate (Pt/Ce-Zr-SO42-) catalysts were prepared by wetness impregnation. Catalytic activities were evaluated from the combustion of propene and CO. Sulfate (SO42-) addition improved the catalytic activity significantly. When using Pt/Ce-Zr-SO42- with 10 wt% SO42-, the temperature for 90% conversion of propene and CO decreased by 75℃ compared with Pt/Ce-Zr. The conversion exceeded 95% at 240℃ even after 0.02% sulfur dioxide poisoning for 20 h. Temperature-programmed desorption of CO and X-ray photoelectron spectroscopy analyses revealed an improvement in Pt dispersion onto the Ce-Zr-SO42- support, and the increased number of Pt particles built up more Pt&+-(SO42-)&- couples, which resulted in excellent activity. The increased total acidity and new Brönsted acid sites on the surface provided the Pt/Ce-Zr-SO42- with good sulfur resistance.

催化学报

Chinese Journal of
Catalysis
Started in 1980
Issues per year: 12
Supervised by
Chinese Academy of Sciences
Sponsored by
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, and the Chinese Chemical Society

 

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Editors-in-Chief
Can Li, Tao Zhang
ISSN 0253-9837
CODEN THHPD3
CN 21-1195/O6
Domestic code number
8-93

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