WorldWideScience

Sample records for carbon catalyst properties

  1. Carbon quantum dots with photo-generated proton property as efficient visible light controlled acid catalyst

    Science.gov (United States)

    Li, Haitao; Liu, Ruihua; Kong, Weiqian; Liu, Juan; Liu, Yang; Zhou, Lei; Zhang, Xing; Lee, Shuit-Tong; Kang, Zhenhui

    2013-12-01

    Developing light-driven acid catalyst will be very meaningful for the controlled-acid catalytic processes towards a green chemical industry. Here, based on scanning electrochemical microscopy (SECM) and ΔpH testing, we demonstrate that the 5-10 nm carbon quantum dots (CQDs) synthesized by electrochemical ablation of graphite have strong light-induced proton properties under visible light in solution, which can be used as an acid catalyst. The 5-10 nm CQDs' catalytic activity is strongly dependent on the illumination intensity and the temperature of the reaction system. As an effective visible light driven and controlled acid-catalyst, 5-10 nm CQDs can catalyze a series of organic reactions (esterification, Beckmann rearrangement and aldol condensation) with high conversion (34.7-46.2%, respectively) in water solution under visible light, while the 1-4 nm CQDs and 10-2000 nm graphite do not have such excellent catalytic activity. The use of 5-10 nm CQDs as a light responsive and controllable photocatalyst is truly a novel application of carbon-based nanomaterials, which may significantly push research in the current catalytic industry, environmental pollution and energy issues.Developing light-driven acid catalyst will be very meaningful for the controlled-acid catalytic processes towards a green chemical industry. Here, based on scanning electrochemical microscopy (SECM) and ΔpH testing, we demonstrate that the 5-10 nm carbon quantum dots (CQDs) synthesized by electrochemical ablation of graphite have strong light-induced proton properties under visible light in solution, which can be used as an acid catalyst. The 5-10 nm CQDs' catalytic activity is strongly dependent on the illumination intensity and the temperature of the reaction system. As an effective visible light driven and controlled acid-catalyst, 5-10 nm CQDs can catalyze a series of organic reactions (esterification, Beckmann rearrangement and aldol condensation) with high conversion (34

  2. Influence of Catalyst and Polymerization Conditions on the Properties of 1,3-Trimethylene Carbonate and ε-Caprolactone Copolymers

    NARCIS (Netherlands)

    Pego, Ana Paula; Zhong, Zhiyuan; Dijkstra, Pieter J.; Grijpma, Dirk W.; Feijen, Jan

    2003-01-01

    The influence of the catalyst/initiator system and polymerization conditions on the microstructure and physical properties of copolymers of equimolar amounts of 1,3-trimethylene carbonate (TMC) and -caprolactone (CL) was studied. Statistical copolymers were prepared in the presence of stannous octoa

  3. Microwave Properties of Carbon Nanotubes Grown by Pyrolysis of Ethanol on Nickel Catalyst

    Directory of Open Access Journals (Sweden)

    V.V. Rodionov

    2014-07-01

    Full Text Available The efficiency of carbon nanotubes produced by CVD-method on a nickel catalyst at a protection from microwave radiation is shown. These data are confirmed by scanning electron microscopy, energy dispersive X-ray analysis and spectral analysis of the microwave radiation in the frequency range 26-40 GHz. The observed value of the transmission coefficient S21, up to – 42.7 dB, is in agreement with considered possible absorption mechanisms of electromagnetic wave energy in carbon nanoscale systems “CNT-nickel nanoparticles”. The application of carbon powder materials in shielding of electromagnetic radiation has been theoretically justified.

  4. Ni-SiO₂ catalysts for the carbon dioxide reforming of methane: varying support properties by flame spray pyrolysis.

    Science.gov (United States)

    Lovell, Emma C; Scott, Jason; Amal, Rose

    2015-01-01

    Silica particles were prepared by flame spray pyrolysis (FSP) as a support for nickel catalysts. The impact of precursor feed rate (3, 5 and 7 mL/min) during FSP on the silica characteristics and the ensuing effect on catalytic performance for the carbon dioxide, or dry, reforming of methane (DRM) was probed. Increasing the precursor feed rate: (i) progressively lowered the silica surface area from ≈340 m2/g to ≈240 m2/g; (ii) altered the silanol groups on the silica surface; and (iii) introduced residual carbon-based surface species to the sample at the highest feed rate. The variations in silica properties altered the (5 wt %) nickel deposit characteristics which in turn impacted on the DRM reaction. As the silica surface area increased, the nickel dispersion increased which improved catalyst performance. The residual carbon-based species also appeared to improve nickel dispersion, and in turn catalyst activity, although not to the same extent as the change in silica surface area. The findings illustrate both the importance of silica support characteristics on the catalytic performance of nickel for the DRM reaction and the capacity for using FSP to control these characteristics.

  5. Ni-SiO2 Catalysts for the Carbon Dioxide Reforming of Methane: Varying Support Properties by Flame Spray Pyrolysis

    Directory of Open Access Journals (Sweden)

    Emma C. Lovell

    2015-03-01

    Full Text Available Silica particles were prepared by flame spray pyrolysis (FSP as a support for nickel catalysts. The impact of precursor feed rate (3, 5 and 7 mL/min during FSP on the silica characteristics and the ensuing effect on catalytic performance for the carbon dioxide, or dry, reforming of methane (DRM was probed. Increasing the precursor feed rate: (i progressively lowered the silica surface area from ≈340 m2/g to ≈240 m2/g; (ii altered the silanol groups on the silica surface; and (iii introduced residual carbon-based surface species to the sample at the highest feed rate. The variations in silica properties altered the (5 wt % nickel deposit characteristics which in turn impacted on the DRM reaction. As the silica surface area increased, the nickel dispersion increased which improved catalyst performance. The residual carbon-based species also appeared to improve nickel dispersion, and in turn catalyst activity, although not to the same extent as the change in silica surface area. The findings illustrate both the importance of silica support characteristics on the catalytic performance of nickel for the DRM reaction and the capacity for using FSP to control these characteristics.

  6. Ni-SiO₂ catalysts for the carbon dioxide reforming of methane: varying support properties by flame spray pyrolysis.

    Science.gov (United States)

    Lovell, Emma C; Scott, Jason; Amal, Rose

    2015-01-01

    Silica particles were prepared by flame spray pyrolysis (FSP) as a support for nickel catalysts. The impact of precursor feed rate (3, 5 and 7 mL/min) during FSP on the silica characteristics and the ensuing effect on catalytic performance for the carbon dioxide, or dry, reforming of methane (DRM) was probed. Increasing the precursor feed rate: (i) progressively lowered the silica surface area from ≈340 m2/g to ≈240 m2/g; (ii) altered the silanol groups on the silica surface; and (iii) introduced residual carbon-based surface species to the sample at the highest feed rate. The variations in silica properties altered the (5 wt %) nickel deposit characteristics which in turn impacted on the DRM reaction. As the silica surface area increased, the nickel dispersion increased which improved catalyst performance. The residual carbon-based species also appeared to improve nickel dispersion, and in turn catalyst activity, although not to the same extent as the change in silica surface area. The findings illustrate both the importance of silica support characteristics on the catalytic performance of nickel for the DRM reaction and the capacity for using FSP to control these characteristics. PMID:25774491

  7. Effects of reaction conditions on hydrogen production and carbon nanofiber properties generated by methane decomposition in a fixed bed reactor using a NiCuAl catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Suelves, I.; Pinilla, J.L.; Lazaro, M.J.; Moliner, R. [Instituto de Carboquimica CSIC, Miguel Luesma Castan, 4, 50015 Zaragoza (Spain); Palacios, J.M. [Instituto de Catalisis y Petroleoquimica, CSIC, Cantoblanco, Marie Curie 2, 28049 Madrid (Spain)

    2009-07-01

    In this paper, the results obtained in the catalytic decomposition of methane in a fixed bed reactor using a NiCuAl catalyst prepared by the fusion method are presented. The influences of reaction temperature and space velocity on hydrogen concentration in the outlet gases, as well as on the properties of the carbon produced, have been investigated. Reaction temperature and the space velocity both increase the reaction rate of methane decomposition, but also cause an increase in the rate of catalyst deactivation. Under the operating conditions used, the carbon product is mainly deposited as nanofibers with textural properties highly correlated with the degree of crystallinity. (author)

  8. Graphitic Carbon Nitride Supported Catalysts for Polymer Electrolyte Fuel Cells.

    Science.gov (United States)

    Mansor, Noramalina; Jorge, A Belen; Corà, Furio; Gibbs, Christopher; Jervis, Rhodri; McMillan, Paul F; Wang, Xiaochen; Brett, Daniel J L

    2014-04-01

    Graphitic carbon nitrides are investigated for developing highly durable Pt electrocatalyst supports for polymer electrolyte fuel cells (PEFCs). Three different graphitic carbon nitride materials were synthesized with the aim to address the effect of crystallinity, porosity, and composition on the catalyst support properties: polymeric carbon nitride (gCNM), poly(triazine) imide carbon nitride (PTI/Li(+)Cl(-)), and boron-doped graphitic carbon nitride (B-gCNM). Following accelerated corrosion testing, all graphitic carbon nitride materials are found to be more electrochemically stable compared to conventional carbon black (Vulcan XC-72R) with B-gCNM support showing the best stability. For the supported catalysts, Pt/PTI-Li(+)Cl(-) catalyst exhibits better durability with only 19% electrochemical surface area (ECSA) loss versus 36% for Pt/Vulcan after 2000 scans. Superior methanol oxidation activity is observed for all graphitic carbon nitride supported Pt catalysts on the basis of the catalyst ECSA.

  9. Effect of the functional groups of carbon on the surface and catalytic properties of Ru/C catalysts for hydrogenolysis of glycerol

    Energy Technology Data Exchange (ETDEWEB)

    Gallegos-Suarez, E. [Departamento de Química Inorgánica y Técnica, Facultad de Ciencias, UNED, Paseo Senda del Rey n° 9, 28040 Madrid (Spain); Instituto de Catálisis y Petroleoquímica, CSIC, Marie Curie n° 2, L-10, 28049 Madrid (Spain); Pérez-Cadenas, M. [Instituto de Catálisis y Petroleoquímica, CSIC, Marie Curie n° 2, L-10, 28049 Madrid (Spain); Guerrero-Ruiz, A. [Instituto de Catálisis y Petroleoquímica, CSIC, Marie Curie n° 2, L-10, 28049 Madrid (Spain); Unidad Asociada UNED ICP-CSIC, Group Design and Applied Heterogeneous Catalysis (Spain); Rodriguez-Ramos, I. [Departamento de Química Inorgánica y Técnica, Facultad de Ciencias, UNED, Paseo Senda del Rey n° 9, 28040 Madrid (Spain); Unidad Asociada UNED ICP-CSIC, Group Design and Applied Heterogeneous Catalysis (Spain); Arcoya, A., E-mail: aarcoya@icp.csic.es [Departamento de Química Inorgánica y Técnica, Facultad de Ciencias, UNED, Paseo Senda del Rey n° 9, 28040 Madrid (Spain); Unidad Asociada UNED ICP-CSIC, Group Design and Applied Heterogeneous Catalysis (Spain)

    2013-12-15

    Ruthenium catalysts supported on activated carbons, original (AC) and treated with nitric acid (AC-Ox) were prepared by incipient wetness impregnation from either chloride (Cl) or nitroxyl nitrate (n) precursors. These catalysts were characterized by TG, XPS, TEM, TPD-MS and CO adsorption microcalorimetry and evaluated in the hydrogenolysis of glycerol in the liquid phase, at 453 K and 8 MPa. Studies by TEM show that ruthenium particles supported on AC-Ox are larger than on AC, without any effect of the nature of the metal precursor. However, adsorption of CO on the ex-chloride catalysts is inhibited in comparison with that of the ex-nitroxyl nitrate catalysts. Catalysts characterization by TG, TPD-MS and XPS reveals that the nitric acid treatment and the nitroxyl nitrate precursor generate oxygenated groups on the carbon surface, which provide acid properties to the catalysts, although they are partly destroyed during the reduction treatment applied to the catalysts. The sequence of the overall TOF, Ru(Cl)/AC < Ru(n)/AC < Ru(Cl)/AC-Ox ≈ Ru(n)/AC-Ox, reasonably parallels the population increase of surface acid groups. Participation of the -COOH groups in the transformation of glycerol into 1,2-propanediol is verified by using the admixture Ru(Cl)/AC+AC-Ox as catalyst. In this case, since AC-Ox was not thermally treated and no loss of oxygenated groups occurred, TOF and selectivity toward 1,2-propanediol improve in comparison with those of the more active catalysts.

  10. Effect of the functional groups of carbon on the surface and catalytic properties of Ru/C catalysts for hydrogenolysis of glycerol

    Science.gov (United States)

    Gallegos-Suarez, E.; Pérez-Cadenas, M.; Guerrero-Ruiz, A.; Rodriguez-Ramos, I.; Arcoya, A.

    2013-12-01

    Ruthenium catalysts supported on activated carbons, original (AC) and treated with nitric acid (AC-Ox) were prepared by incipient wetness impregnation from either chloride (Cl) or nitroxyl nitrate (n) precursors. These catalysts were characterized by TG, XPS, TEM, TPD-MS and CO adsorption microcalorimetry and evaluated in the hydrogenolysis of glycerol in the liquid phase, at 453 K and 8 MPa. Studies by TEM show that ruthenium particles supported on AC-Ox are larger than on AC, without any effect of the nature of the metal precursor. However, adsorption of CO on the ex-chloride catalysts is inhibited in comparison with that of the ex-nitroxyl nitrate catalysts. Catalysts characterization by TG, TPD-MS and XPS reveals that the nitric acid treatment and the nitroxyl nitrate precursor generate oxygenated groups on the carbon surface, which provide acid properties to the catalysts, although they are partly destroyed during the reduction treatment applied to the catalysts. The sequence of the overall TOF, Ru(Cl)/AC < Ru(n)/AC < Ru(Cl)/AC-Ox ≈ Ru(n)/AC-Ox, reasonably parallels the population increase of surface acid groups. Participation of the sbnd COOH groups in the transformation of glycerol into 1,2-propanediol is verified by using the admixture Ru(Cl)/AC+AC-Ox as catalyst. In this case, since AC-Ox was not thermally treated and no loss of oxygenated groups occurred, TOF and selectivity toward 1,2-propanediol improve in comparison with those of the more active catalysts.

  11. Effect of the functional groups of carbon on the surface and catalytic properties of Ru/C catalysts for hydrogenolysis of glycerol

    International Nuclear Information System (INIS)

    Ruthenium catalysts supported on activated carbons, original (AC) and treated with nitric acid (AC-Ox) were prepared by incipient wetness impregnation from either chloride (Cl) or nitroxyl nitrate (n) precursors. These catalysts were characterized by TG, XPS, TEM, TPD-MS and CO adsorption microcalorimetry and evaluated in the hydrogenolysis of glycerol in the liquid phase, at 453 K and 8 MPa. Studies by TEM show that ruthenium particles supported on AC-Ox are larger than on AC, without any effect of the nature of the metal precursor. However, adsorption of CO on the ex-chloride catalysts is inhibited in comparison with that of the ex-nitroxyl nitrate catalysts. Catalysts characterization by TG, TPD-MS and XPS reveals that the nitric acid treatment and the nitroxyl nitrate precursor generate oxygenated groups on the carbon surface, which provide acid properties to the catalysts, although they are partly destroyed during the reduction treatment applied to the catalysts. The sequence of the overall TOF, Ru(Cl)/AC < Ru(n)/AC < Ru(Cl)/AC-Ox ≈ Ru(n)/AC-Ox, reasonably parallels the population increase of surface acid groups. Participation of the -COOH groups in the transformation of glycerol into 1,2-propanediol is verified by using the admixture Ru(Cl)/AC+AC-Ox as catalyst. In this case, since AC-Ox was not thermally treated and no loss of oxygenated groups occurred, TOF and selectivity toward 1,2-propanediol improve in comparison with those of the more active catalysts.

  12. Carbon Nanofibers as Catalyst Support for Noble Metals

    OpenAIRE

    Toebes, M.L.

    2004-01-01

    In the quest for new and well-defined support materials for heterogeneous catalysts we explored the potential of carbon nanofibers (CNF). CNF belongs to the by now extensive family of synthetic graphite-like carbon materials with advantageous and tunable physico-chemical properties. Aim of the work described in this thesis has been the exploration of the potential of CNF as catalyst support material, notably for platinum and ruthenium, and its role in the performance of these catalysts in hyd...

  13. Carbon Fiber Composite Monoliths as Catalyst Supports

    Energy Technology Data Exchange (ETDEWEB)

    Contescu, Cristian I [ORNL; Gallego, Nidia C [ORNL; Pickel, Joseph M [ORNL; Blom, Douglas Allen [ORNL; Burchell, Timothy D [ORNL

    2006-01-01

    Carbon fiber composite monoliths are rigid bodies that can be activated to a large surface area, have tunable porosity, and proven performance in gas separation and storage. They are ideal as catalyst supports in applications where a rigid support, with open structure and easy fluid access is desired. We developed a procedure for depositing a dispersed nanoparticulate phase of molybdenum carbide (Mo2C) on carbon composite monoliths in the concentration range of 3 to 15 wt% Mo. The composition and morphology of this phase was characterized using X-ray diffraction and electron microscopy, and a mechanism was suggested for its formation. Molybdenum carbide is known for its catalytic properties that resemble those of platinum group metals, but at a lower cost. The materials obtained are expected to demonstrate catalytic activity in a series of hydrocarbon reactions involving hydrogen transfer. This project demonstrates the potential of carbon fiber composite monoliths as catalyst supports.

  14. Carbon Fiber Composite Monoliths for Catalyst Supports

    Energy Technology Data Exchange (ETDEWEB)

    Contescu, Cristian I [ORNL; Gallego, Nidia C [ORNL; Pickel, Joseph M [ORNL; Blom, Douglas Allen [ORNL; Burchell, Timothy D [ORNL

    2006-01-01

    Carbon fiber composite monoliths are rigid bodies that can be activated to a large surface area, have tunable porosity, and proven performance in gas separation and storage. They are ideal as catalyst supports in applications where a rigid support, with open structure and easy fluid access is desired. We developed a procedure for depositing a dispersed nanoparticulate phase of molybdenum carbide (Mo2C) on carbon composite monoliths in the concentration range of 3 to 15 wt% Mo. The composition and morphology of this phase was characterized using X-ray diffraction and electron microscopy, and a mechanism was suggested for its formation. Molybdenum carbide is known for its catalytic properties that resemble those of platinum group metals, but at a lower cost. The materials obtained are expected to demonstrate catalytic activity in a series of hydrocarbon reactions involving hydrogen transfer. This project demonstrates the potential of carbon fiber composite monoliths as catalyst supports.

  15. PREPARATION OF MESOPOROUS CARBON BY CARBON DIOXIDE ACTIVATION WITH CATALYST

    Institute of Scientific and Technical Information of China (English)

    W.Z.Shen; A.H.Lu; J.T.Zheng

    2002-01-01

    A mesoporous activated carbon (AC) can be successfully prepared by catalytic activa-tion with carbon dioxide. For iron oxide as catalyst, there were two regions of mesoporesize distribution, i.e. 2-5nm and 30-70nm. When copper oxide or magnesium oxidecoexisted with iron oxide as composite catalyst, the content of pores with sizes of 2-5nm was decreased, while the pores with 30 70nm were increased significantly. Forcomparison, AC reactivated by carbon dioxide directly was also investigated. It wasshown that the size of mesopores of the resulting AC concentrated in 2-5nm with lessvolume. The adsorption of Congo red was tested to evaluate the property of the result-ing AC. Furthermore, the factors affecting pore size distribution and the possibility ofmesopore formation were discussed.

  16. Graphitic Carbon Nitride Supported Catalysts for Polymer Electrolyte Fuel Cells.

    OpenAIRE

    Mansor, N.; Jorge, A. B.; Corà, F.; Gibbs, C.; Jervis, R.; Mcmillan, P. F.; X. Wang; Brett, D. J.

    2014-01-01

    Graphitic carbon nitrides are investigated for developing highly durable Pt electrocatalyst supports for polymer electrolyte fuel cells (PEFCs). Three different graphitic carbon nitride materials were synthesized with the aim to address the effect of crystallinity, porosity, and composition on the catalyst support properties: polymeric carbon nitride (gCNM), poly(triazine) imide carbon nitride (PTI/Li(+)Cl(-)), and boron-doped graphitic carbon nitride (B-gCNM). Following accelerated corrosion...

  17. Synthesis of carbon nanotubes with Ni/CNTs catalyst

    Institute of Scientific and Technical Information of China (English)

    LI; Chunhua; (李春华); YAO; Kefu; (姚可夫); RUAN; Dianbo; (阮殿波); LIANG; Ji; (梁; 吉); XU; Cailu; (徐才录); WU; Dehai; (吴德海)

    2003-01-01

    Carbon nanotubes (CNTs), owing to their large specific area, good chemical stability and modifiable surface properties after acidic or basic treatment, can be used as catalytic support materials. In this paper, the activities and selectivities of two catalysts, i. e. Ni catalyst supported by carbon nanotubes (Ni/CNTs) and that supported by diatomite (Ni/SiO2), are compared. It is found that the quality of the carbon nanotubes synthesized by the two catalysts is similar, but the yield of the former is 1.5 times higher than that of the latter. The excellent performance of the Ni/CNTs catalyst should be ascribed to the larger specific surface area and proper pore distribution and the structure of the carbon nanotube support.

  18. Carbon Nanofibers as Catalyst Support for Noble Metals

    NARCIS (Netherlands)

    Toebes, M.L.

    2004-01-01

    In the quest for new and well-defined support materials for heterogeneous catalysts we explored the potential of carbon nanofibers (CNF). CNF belongs to the by now extensive family of synthetic graphite-like carbon materials with advantageous and tunable physico-chemical properties. Aim of the work

  19. Thermodynamic Properties of Supported Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Gorte, Raymond J.

    2014-03-26

    The goals of this work were to develop Coulometric Titration as a method for characterizing the thermodynamic redox properties of oxides and to apply this technique to the characterization of ceria- and vanadia-based catalysts. The redox properties of ceria and vanadia are a major part of what makes these materials catalytically active but their properties are also dependent on their structure and the presence of other oxides. Quantifying these properties through the measurement of oxidation energetics was the goal of this work.

  20. Immobilized Ruthenium Catalyst for Carbon Dioxide Hydrogenation

    Institute of Scientific and Technical Information of China (English)

    Ying Min YU; Jin Hua FEI; Yi Ping ZHANG; Xiao Ming ZHENG

    2006-01-01

    Three kinds of cross linked polystyrene resin (PS) supported ruthenium complexes were developed as catalysts for the synthesis of formic acid from carbon dioxide hydrogenation. Many factors, such as the functionalized supports, solvents and ligands, could influence their activities and reuse performances greatly. These immobilized catalysts also offer the industrial advantages such as easy separation.

  1. Active carbon catalyst for heavy oil upgrading

    Energy Technology Data Exchange (ETDEWEB)

    Fukuyama, Hidetsugu; Terai, Satoshi [Technology Research Center, Toyo Engineering Corporation, 1818 Azafujimi, Togo, Mobara-shi, Chiba 297-00017 (Japan); Uchida, Masayuki [Business Planning and Exploring Department, Overseas Business Development and Marketing Division, Toyo Engineering Corporation, 2-8-1 Akanehama, Narashino-shi, Chiba 275-0024 (Japan); Cano, Jose L.; Ancheyta, Jorge [Maya Crude Treatment Project, Instituto Mexicano del Petroleo, Eje Central Lazaro Cardenas No. 152, Col. San Bartolo Atepehuacan, Mexico D.F. 07730 (Mexico)

    2004-11-24

    The active carbon (AC) catalyst was studied by hydrocracking of Middle Eastern vacuum residue (VR) for heavy oil upgrading. It was observed that the active carbon has the affinity to heavy hydrocarbon compounds and adsorption selectivity to asphaltenes, and exhibits better ability to restrict the coke formation during the hydrocracking reaction of VR. The mesopore of active carbon was thought to play an important role for effective conversion of heavy hydrocarbon compounds into lighter fractions restricting carbon formation. The performance of the AC catalyst was examined by continuous hydrocracking by CSTR for the removal of such impurities as sulfur and heavy metals (nickel and vanadium), which are mostly concentrated in the asphaltenes. The AC catalyst was confirmed to be very effective for the removal of heavy metals from Middle Eastern VR, Maya/Istmo VR and Maya VR. The extruded AC catalysts were produced by industrial manufacturing method. The application test of the extruded AC catalyst for ebullating-bed reactor as one of the commercially applicable reactors was carried out at the ebullating-bed pilot plant for 500h. The ebullition of the extruded AC catalyst was successfully traced and confirmed by existing {gamma}-ray density meter. The extruded AC catalyst showed stable performance with less sediment formation at an equivalent conversion by conventional alumina catalyst at commercial ebullating-bed unit. The degradation of the AC catalyst at the aging test was observed to be less than that of the conventional alumina catalyst. Thus, the AC catalyst was confirmed to be effective and suitable for upgrading of heavy oil, especially such heavy oils as Maya, which contains much heavy metals.

  2. States of Carbon Nanotube Supported Mo-Based HDS Catalysts

    Institute of Scientific and Technical Information of China (English)

    Hongyan Shang; Chenguang Liu; Yongqiang Xu; Jieshan Qiu; Fei Wei

    2006-01-01

    The dispersion of the active phase and loading capacity of the Mo species on carbon nanotube (CNT) was studied by the XRD technique. The reducibility properties of Co-Mo catalysts in the oxide state over CNTs were investigated by TPR, while the sulfided Co-Mo/CNT catalysts were characterized by means of the XRD and LRS techniques. The activity and selectivity with respect to the hydrodesulfurization (HDS) performances on carbon nanotube supported Co-Mo catalysts were evaluated. It was found that the main active molybdenum species in the oxide state MoO3/CNT catalysts were MoO2, but not MoO3, as generally expected. The maximum loading before the formation of the bulk phase was lower than 6% (percent by mass, based on MoO3). TPR studies revealed that the active species in the oxide state Co-Mo/CNT catalysts were reduced more easily at relatively lower temperatures in comparison to those of the Co-Mo/γ-Al2O3 catalysts, indicating that the CNT support promoted or favored the reduction of the active species. The active species of a Co-Mo-0.7/CNT catalyst were more easily reduced than those of the Co-Mo/CNT catalysts with Co/Mo atomic ratios of 0.2, 0.35, and 0.5, respectively, suggesting that the Co/Mo atomic ratio has a great effect on the reducibility of the active species. It was found that the incorporation of cobalt improved the dispersion of the molybdenum species on the support, and a phenomenon of mobilization and re-dispersion had occurred during the sulfurization process, resulting in low valence state Mo3S4 and Co-MoS2.17 active phases. HDS measurements showed that the Co-Mo/CNT catalysts were more active than the Co-Mo/γ-Al2O3 ones for the desulfurization of DBT, and the hydrogenolysis/hydrogenation selectivity of the Co-Mo/CNT catalysts was also much higher than those of the Co-Mo/γ-Al2O3. The Co-Mo/CNT catalyst with a Co/Mo atomic ratio of 0.7 showed the highest activity, whereas the catalyst with a Co/Mo atomic ratio of 0.35 had the highest selectivity.

  3. Catalysts for Efficient Production of Carbon Nanotubes

    Science.gov (United States)

    Sun, Ted X.; Dong, Yi

    2009-01-01

    Several metal alloys have shown promise as improved catalysts for catalytic thermal decomposition of hydrocarbon gases to produce carbon nanotubes (CNTs). Heretofore almost every experiment on the production of carbon nanotubes by this method has involved the use of iron, nickel, or cobalt as the catalyst. However, the catalytic-conversion efficiencies of these metals have been observed to be limited. The identification of better catalysts is part of a continuing program to develop means of mass production of high-quality carbon nanotubes at costs lower than those achieved thus far (as much as $100/g for purified multi-wall CNTs or $1,000/g for single-wall CNTs in year 2002). The main effort thus far in this program has been the design and implementation of a process tailored specifically for high-throughput screening of alloys for catalyzing the growth of CNTs. The process includes an integral combination of (1) formulation of libraries of catalysts, (2) synthesis of CNTs from decomposition of ethylene on powders of the alloys in a pyrolytic chemical-vapor-decomposition reactor, and (3) scanning- electron-microscope screening of the CNTs thus synthesized to evaluate the catalytic efficiencies of the alloys. Information gained in this process is put into a database and analyzed to identify promising alloy compositions, which are to be subjected to further evaluation in a subsequent round of testing. Some of these alloys have been found to catalyze the formation of carbon nano tubes from ethylene at temperatures as low as 350 to 400 C. In contrast, the temperatures typically required for prior catalysts range from 550 to 750 C.

  4. Functionalization of Carbon Nanofibres Obtained by Floating Catalyst Method

    Directory of Open Access Journals (Sweden)

    Adolfo Fernández

    2015-01-01

    Full Text Available The excellent physicochemical and electrical properties of carbon nanofibres (CNF combined with the possibility of being produced at industrial scale at reasonable costs have promoted the interest in their use in very diverse areas. However, there are still some drawbacks that must be solved in order to optimize their set of properties such as the presence of impurities or the imperfections in the crystalline structure. In this work, different modification treatments of CNFs produced by the floating catalyst method have been studied. Three types of modification processes have been explored that can be grouped as mechanical, thermal, and chemical functionalization processes. Mechanical processing has allowed solving the agglomeration problem related to CNFs produced by floating catalyst method and the resulting modified product ensures the secure handling of carbon nanofibres. Thermal and chemical treatments lead to purer and more crystalline products by removing catalyst impurities and amorphous carbon. Functionalization processes explored in this work open the possibility of customized posttreatment of carbon nanofibres according to the desired requirements.

  5. XPS studies of Pt catalysts supported on porous carbon

    Science.gov (United States)

    Tyagi, Deepak; Varma, Salil; Bharadwaj, S. R.

    2016-05-01

    Pt catalysts supported on porous carbon were prepared by hard templating route and used for HI decomposition reaction of Sulfur Iodine thermochemical cycle. These catalysts were characterized by X-ray photoelectron spectroscopy for oxidation state of platinum as well as nature of carbon present in the catalysts. It was found that platinum is present in metallic state and carbon is present in both sp2 and sp3 hybridization states. The catalysts were evaluated for their activity and stability for liquid phase HI decomposition reaction and it was observed that mesoporous carbon based catalysts were more active and stable under the reaction conditions.

  6. The electrocatalytic properties of carbon supported PtRu/C nanoalloys in oxidation of small organic molecules: Comparison with Pt/C catalyst

    Directory of Open Access Journals (Sweden)

    Lović Jelena D.

    2012-01-01

    Full Text Available The electrocatalytic activity of carbon supported PtRu/C catalysts, with different composition, toward the electrooxidation of methanol, CO and formic acid were examined in acid and alkaline solution at ambient temperature using thin-film rotating disk electrode (RDE method and compared with activity of Pt/C. The catalysts were characterized by XRD, AFM and STM techniques. XRD pattern revealed that PtRu-1/C catalyst is consisted of two structures e.g. Pt-Ru-fcc and Ru-hcp (the solid solution of Ru in Pt and the small amount of Ru or solid solution of Pt in Ru, as opposed to PtRu-2/C catalyst which is consisted of one structure mostly, Pt-Ru-fcc. According to STM images, PtRu as well as Pt, particles size were between 2 and 6 nm, which is in a good agreement with the mean particles size determined by XRD. To establish the activity and stability of the catalysts potentiodynamic and quasi steady-state measurements were performed. It was found that the activity of Pt and PtRu for CO and methanol oxidation is a strong function of pH of solution. The kinetics are much higher in alkaline than in acid solution and the difference between Pt/C and PtRu/C is much less pronounced in alkaline media. Results presented in this work indicate that activity of PtRu catalysts depends on catalyst composition, e.g. on Pt/Ru atomic ratio, as well as on alloying degree of catalysts. Comparison of CO, methanol and formic acid oxidation on PtRu-2/C, PtRu-1/C and Pt/C catalysts revealed that PtRu-2/C is the most active one. It was shown that the PtRu-2/C catalyst, due to fact that it is consisted of only one phase, with high alloying degree, through the bifunctional mechanism improved by electronic effect, achieve the activity two times higher related to PtRu-1/C in the oxidation of all organic molecules investigated, and about three times higher compared to Pt/C in the oxidation of methanol and CO, and five times higher in formic acid oxidation.

  7. Nitrogen-doped carbon nanotubes on silicon carbide as a metal-free catalyst

    Institute of Scientific and Technical Information of China (English)

    Cuong Duong-Viet; Housseinou Ba; Yuefeng Liu; Lai Truong-Phuoc; Jean-Mario Nhut; Cuong Pham-Huu

    2014-01-01

    A hierarchical metal-free catalyst consisting of nitrogen-doped carbon nanotubes decorated onto a silicon carbide (N-CNTs/SiC) macroscopic host structure was prepared. The influence of N-CNTs incorporation on the physical properties of the support was evaluated using different characteriza-tion techniques. The catalyst was tested as a metal-free catalyst in the selective oxidation of H2S and steam-free dehydrogenation of ethylbenzene. The N-CNTs/SiC catalyst exhibited extremely good desulfurization performance compared to a Fe2O3/SiC catalyst under less conducive reaction condi-tions such as low temperature, high space velocity, and a low O2-to-H2S molar ratio. For the dehy-drogenation of ethylbenzene, a higher dehydrogenation activity was obtained with the N-CNTs/SiC catalyst compared to a commercial K-Fe/Al2O3 catalyst. The N-CNTs/SiC catalyst also displayed good stability as a function of time on stream for both reactions, which was attributed to the strong anchoring of the nitrogen dopant in the carbon matrix. The extrudate shape of the SiC support al-lowed the direct macroscopic shaping of the catalyst for use in a conventional fixed-bed reactor without the problems of catalyst handling, transportation, and pressure drop across the catalyst bed that are encountered with nanoscopic carbon-based catalysts.

  8. Allotropic Carbon Nanoforms as Advanced Metal-Free Catalysts or as Supports

    Directory of Open Access Journals (Sweden)

    Hermenegildo Garcia

    2014-01-01

    Full Text Available This perspective paper summarizes the use of three nanostructured carbon allotropes as metal-free catalysts (“carbocatalysts” or as supports of metal nanoparticles. After an introductory section commenting the interest of developing metal-free catalysts and main features of carbon nanoforms, the main body of this paper is focused on exemplifying the opportunities that carbon nanotubes, graphene, and diamond nanoparticles offer to develop advanced catalysts having active sites based on carbon in the absence of transition metals or as large area supports with special morphology and unique properties. The final section provides my personal view on future developments in this field.

  9. CARBON NANOTUBES VIA METHANE DECOMPOSITION ON AN ALUMINA SUPPORTED COBALT AEROGEL CATALYST

    Institute of Scientific and Technical Information of China (English)

    Lingyu Piao; Jiuling Chen; Yongdan Li

    2003-01-01

    An alumina-supported cobalt aerogel catalyst prepared from a sol-gel and a supercritical drying method was used in the catalytic decomposition of methane. The physical-chemical properties of the catalyst were characterized and its activity for methane decomposition was investigated. The effects of calcination and reaction temperatures on the activity of the catalyst and the morphology of the carbon nanotubes produced were discussed. A CoAl2O4 spinel structure formed in the calcined catalyst. The quantity of the nanotubes produced in the reaction increases with the amount of cobalt in the reduced catalyst. A higher reaction temperature leads to a higher reaction rate, though faster deactivation of the catalyst occurs with the change. The carbon nanotubes grown on the catalyst have smooth walls and uniform diameter distribution.

  10. Thief carbon catalyst for oxidation of mercury in effluent stream

    Science.gov (United States)

    Granite, Evan J.; Pennline, Henry W.

    2011-12-06

    A catalyst for the oxidation of heavy metal contaminants, especially mercury (Hg), in an effluent stream is presented. The catalyst facilitates removal of mercury through the oxidation of elemental Hg into mercury (II) moieties. The active component of the catalyst is partially combusted coal, or "Thief" carbon, which can be pre-treated with a halogen. An untreated Thief carbon catalyst can be self-promoting in the presence of an effluent gas streams entrained with a halogen.

  11. States of carbon nanotube supported Mo-based HDS catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Shang, Hongyan; Liu, Chenguang; Xu, Yongqiang [Key Laboratory of Catalysis, CNPC, College of Chemistry and Chemical Engineering, University of Petroleum, Dongying 257061 (China); Qiu, Jieshan [Carbon Research Laboratory, Center for Nano Materials and Science, Dalian University of Technology, 158 Zhongshan Road, P. O. Box 49, Dalian 116012 (China); Wei, Fei [Department of Chemical Engineering, Tsinghua University, Being, 100084 (China)

    2007-02-15

    As HDS catalysts, the supported catalysts including oxide state Mo, Co-Mo and sulfide state Mo on carbon nanotube (CNT) were prepared, while the corresponding supported catalysts on {gamma}-Al{sub 2}O{sub 3} were prepared as comparison. Firstly, the dispersion of the active phase and loading capacity of Mo species on CNT was studied by XRD and the reducibility properties of Co-Mo catalysts in oxide state over CNTs were investigated by TPR while the sulfide Co-Mo/CNT catalysts were characterized by XRD and LRS techniques. Secondly, the activity and selectivity of hydrodesulfurization (HDS) of dibenzothiophene with Co-Mo/CNT and Co-Mo/{gamma}-Al{sub 2}O{sub 3} were studied. It has been found that the main active molybdenum species in the oxide state MoO{sub 3}/CNT catalysts were MoO{sub 2}, rather than MoO{sub 3} as generally expected. The maximum loading before formation of the bulk phase was lower than 6%m (calculated in MoO{sub 3}). The TPR studies revealed that that active species in oxide state Co-Mo/CNT catalysts were more easily reduced at relatively lower temperatures in comparison to those in Co-Mo/{gamma}-Al{sub 2}O{sub 3}, indicating that the CNT support promoted the reduction of active species. Among 0-1.0 Co/Mo atomic ratio on Co-Mo/CNT, 0.7 has the highest reducibility. It shows that the Co/Mo atomic ratio has a great effect on the reducibility of active species on CNT and their HDS activities and that the incorporation of cobalt improved the dispersion of molybdenum species on CNT and mobilization. It was also found that re-dispersion could occur during the sulfiding process, resulting in low valence state Mo{sub 3}S{sub 4} and Co-MoS{sub 2.17} active phases. The HDS of DBT showed that Co-Mo/CNT catalysts were more active than Co-Mo/{gamma}-Al{sub 2}O{sub 3} and the hydrogenolysis/hydrogenation selectivity of Co-Mo/CNT catalyst was also much higher than Co-Mo/{gamma}-Al{sub 2}O{sub 3}. For the Co-Mo/CNT catalysis system, the catalyst with Co/Mo atomic

  12. Magnetism for understanding catalyst analysis of purified carbon nanotubes

    Science.gov (United States)

    Bellouard, Christine; Mercier, Guillaume; Cahen, Sébastien; Ghanbaja, Jaafar; Medjahdi, Ghouti; Gleize, Jérôme; Lamura, Gianrico; Hérold, Claire; Vigolo, Brigitte

    2016-08-01

    The precise quantification of catalyst residues in purified carbon nanotubes is often a major issue in view of any fundamental and/or applicative studies. More importantly, since the best CNTs are successfully grown with magnetic catalysts, their quantification becomes strictly necessary to better understand intrinsic properties of CNT. For these reasons, we have deeply analyzed the catalyst content remained in nickel-yttrium arc-discharge single walled carbon nanotubes purified by both a chlorine-gas phase and a standard acid-based treatment. The study focuses on Ni analysis which has been investigated by transmission electron microscopy, X-ray diffraction, thermogravimetry analysis, and magnetic measurements. In the case of the acid-based treatment, all quantifications result in a decrease of the nanocrystallized Ni by a factor of two. In the case of the halogen gas treatment, analysis and quantification of Ni content is less straightforward: a huge difference appears between X-ray diffraction and thermogravimetry results. Thanks to magnetic measurements, this disagreement is explained by the presence of Ni2+ ions, belonging to NiCl2 formed during the Cl-based purification process. In particular, NiCl2 compound appears under different magnetic/crystalline phases: paramagnetic or diamagnetic, or well intercalated in between carbon sheets with an ordered magnetic phase at low temperature.

  13. Nickel catalysts for internal reforming in molten carbonate fuel cells

    OpenAIRE

    Berger, R.J.; Doesburg, E.B.M.; Ommen, van, B.; Ross, J.R.H.

    1996-01-01

    Natural gas may be used instead of hydrogen as fuel for the molten carbonate fuel cell (MCFC) by steam reforming the natural gas inside the MCFC, using a nickel catalyst (internal reforming). The severe conditions inside the MCFC, however, require that the catalyst has a very high stability. In order to find suitable types of nickel catalysts and to obtain more knowledge about the deactivation mechanism(s) occurring during internal reforming, a series of nickel catalysts was prepared and subj...

  14. Application of aromatization catalyst in synthesis of carbon nanotubes

    Indian Academy of Sciences (India)

    Song Rongjun; Yang Yunpeng; Ji Qing; Li Bin

    2012-02-01

    In a typical chemical vapour deposition (CVD) process for synthesizing carbon nanotubes (CNTs), it was found that the aromatization catalysts could promote effectively the formation of CNT. The essence of this phenomenon was attributed to the fact that the aromatization catalyst can accelerate the dehydrogenation–cyclization and condensation reaction of carbon source, which belongs to a necessary step in the formation of CNTs. In this work, aromatization catalysts, H-beta zeolite, HZSM-5 zeolite and organically modified montmorillonite (OMMT) were chosen to investigate their effects on the formation of multi-walled carbon nanotubes (MWCNTs) via pyrolysis method when polypropylene and 1-hexene as carbon source and Ni2O3 as the charring catalyst. The results demonstrated that the combination of those aromatization catalysts with nickel catalyst can effectively improve the formation of MWCNTs.

  15. Potassium hydroxide catalyst supported on palm shell activated carbon for transesterification of palm oil

    Energy Technology Data Exchange (ETDEWEB)

    Baroutian, Saeid; Aroua, Mohamed Kheireddine; Raman, Abdul Aziz Abdul; Sulaiman, Nik Meriam Nik [Department of Chemical Engineering, Faculty of Engineering, University of Malaya, 50603 Kuala Lumpur (Malaysia)

    2010-11-15

    In this study, potassium hydroxide catalyst supported on palm shell activated carbon was developed for transesterification of palm oil. The Central Composite Design (CCD) of the Response Surface Methodology (RSM) was employed to investigate the effects of reaction temperature, catalyst loading and methanol to oil molar ratio on the production of biodiesel using activated carbon supported catalyst. The highest yield was obtained at 64.1 C reaction temperature, 30.3 wt.% catalyst loading and 24:1 methanol to oil molar ratio. The physical and chemical properties of the produced biodiesel met the standard specifications. This study proves that activated carbon supported potassium hydroxide is an effective catalyst for transesterification of palm oil. (author)

  16. Synthesis and characterization of niobium-promoted cobalt/iron catalysts supported on carbon nanotubes for the hydrogenation of carbon monoxide

    Institute of Scientific and Technical Information of China (English)

    Zahra Gholami; Noor Asmawati Mohd Zabidi; Fatemeh Gholami; Mohammadtaghi Vakili

    2016-01-01

    Bimetallic Co/Fe catalysts supported on carbon nanotubes ( CNTs) were prepared, and niobium ( Nb) was added as promoter to the 70Co:30Fe/CNT catalyst. The physicochemical properties of the catalysts were characterized, and the catalytic performances were analyzed at the same operation conditions (H2:CO (volume ratio)= 2:1, p = 1 MPa, and t = 260℃) in a tubular fixed-bed microreactor system. The addition of Nb to the bimetallic catalyst decreases the average size of the oxide nanoparticles and improves the reducibility of the bimetallic catalyst. Evaluation of the catalyst performance in a Fischer-Tropsch reaction shows that the catalyst results in high selectivity to methane, and the selectivity to C5+ increased slightly in the bimetallic catalyst unlike that in the monometallic catalysts. The addition of 1% Nb to the bimetallic catalyst increases CO conversion and selectivity to C5+. Meanwhile, a decrease in methane selectivity is observed.

  17. Design of stable catalysts for methane-carbon dioxide reforming

    NARCIS (Netherlands)

    Lercher, J.A.; Bitter, J.H.; Hally, W.; Niessen, W.; Seshan, K.

    2001-01-01

    The activity and stability of catalysts for methane-carbon dioxide reforming depend subtly upon the support and the active metal. Methane decomposes to carbon and hydrogen, forming carbon on the oxide support and the metal. Carbon on the metal is reactive and can be oxidized to CO by oxygen from dis

  18. Study on the oxygen adsorption property of nitrogen-containing metal-free carbon-based cathode catalysts for oxygen reduction reaction

    International Nuclear Information System (INIS)

    We study the characteristics of oxygen adsorption on metal-free carbon-based cathode catalysts derived from nitrogen-containing polyamide (PA) and nitrogen-free phenolic resin (PhRs). Electrochemical analysis and Raman spectroscopy showed higher 2-electron oxygen reduction reaction (ORR) activity and more defect sites in PA than PhRs. The increase in the amount of adsorbed oxygen in PA was also identified by oxygen adsorption isotherms. In situ X-ray photoelectron spectroscopy revealed that graphite-like nitrogen contributes to oxygen adsorption and C=O components are dominant in PA. These experimental results indicate that the adsorbed C=O components near the graphite-like nitrogen can be assigned as active sites for 2-electron ORR.

  19. Improvements in NOx reduction by carbon using bimetallic catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Illan-Gomez, M.J.; Brandan, S.; Salinas-Martinez de Lecea, C.; Linares-Solano, A. [Universidad de Alicante, Alicante (Spain). Departamento de Quimica Inorganica

    2001-11-30

    A catalysis of the C-NOx reaction has been studied to optimize the composition of the catalysts in order to decrease the carbon consumption by oxygen. Both the metal content and the composition of the catalysts have been investigated. The activity of bimetallic (KNi, NiCo and NiCu) catalysts for NOx reduction by carbon has been studied using both isothermal reactions at 300{sup o}C and temperature programmed reaction up to 500{sup o}C. It has been found that the experimental variables (i.e. amount of catalysts and nature of the bimetallic catalysts) determine the selectivity against carbon combustion by oxygen. Thus, it has been observed that the amount of catalyst greatly affects the C-O{sub 2} reaction but only lightly the C-NOx reaction and, consequently, modifies the selectivity of the catalyst for NOx reduction. Among the bimetallic catalysts tested, NiCu catalyst presents the best performance, at a temperature as low as 250{sup o}C, a high de-NOx activity and a high NOx selectivity due to a low carbon burn-off, with the additional advantage of the absence of N{sub 2}O and CO in the reaction products. Thus, the results obtained in this study show, in comparison with our previous results, that better selectivities are achieved. 20 refs., 3 figs., 2 tabs.

  20. Influence of the Synthesis Method for Pt Catalysts Supported on Highly Mesoporous Carbon Xerogel and Vulcan Carbon Black on the Electro-Oxidation of Methanol

    OpenAIRE

    Cinthia Alegre; María Elena Gálvez; Rafael Moliner; María Jesús Lázaro

    2015-01-01

    Platinum catalysts supported on carbon xerogel and carbon black (Vulcan) were synthesized with the aim of investigating the influence of the characteristics of the support on the electrochemical performance of the catalysts. Three synthesis methods were compared: an impregnation method with two different reducing agents, sodium borohydride and formic acid, and a microemulsion method, in order to study the effect of the synthesis method on the physico-chemical properties of the catalysts. X-ra...

  1. Carbon-Supported Silver Catalysts for CO Selective Oxidation in Excess Hydrogen

    Institute of Scientific and Technical Information of China (English)

    Limin Chen; Ding Ma; Barbara Pietruszka; Xinhe Bao

    2006-01-01

    Carbon materials were used as supports for Ag catalysts that are prepared using the conventional wet impregnation method, and their catalytic properties for CO selective oxidation in excess hydrogen at temperatures below 483 K were tested. A variety of techniques, e.g. N2 adsorption, XPS, TPD, UV-Vis DRS, TEM and SEM, were used to determine the influence of physical and chemical properties of the carbon on the properties of Ag catalyst. It was found that defects on the carbon surface served as nucleation sites for silver ions, while functional groups on carbon surface induced their reduction to the metallic form. The formation of silver particles on carbon was governed by homogeneous and/or heterogeneous nucleation during the impregnation and subsequent activation processes. The best catalytic performance was obtained with a Ag/carbon black catalyst with a uniform size distribution of silver nanoparticles (about 12 nm), moderate BET surface area (with a mesoporous structure), and a limited amount of carbon-oxygen groups. The research indicates that carbon materials are potentially good supports for silver catalysts for preferential oxidation of CO in excess hydrogen.

  2. Glow Discharge Plasma-Assisted Preparation of Nickel-Based Catalyst for Carbon Dioxide Reforming of Methane

    Institute of Scientific and Technical Information of China (English)

    Fang Guo; Wei Chu; Jun-qiang Xu; Lin Zhong

    2008-01-01

    A plasma-assisted method was employed to prepare Ni/γ-Al2O3 catalyst for carbon dioxide reforming of methane reaction. The novel catalyst possessed higher activity and better coke-suppression performance than those of the conventional calcination catalyst. To achieve the same CH4 conversion, the conventional catalyst needed higher reaction temperature, about 50 ℃ higher than that of the N2 plasma-treated catalyst.After the evaluation test, the deactivation rate of the novel catalyst was 1.7%, compared with 15.2% for the conventional catalyst. Different from the characterization results of the calcined catalyst, a smaller average pore diameter and a higher specific surface area were obtained for the plasma-treated catalyst.The variations of the reduction peak temperatures and areas indicated that the catalyst reducibility was promoted by plasma assistance. The dispersion of nickel was also remarkably improved, which was helpful for controlling the ensemble size of metal atoms on the catalyst surface. The modification effect of plasmaassisted preparation on the surface property of alumina supported catalyst was speculated to account for the concentration increase of absorbed CO2. An enhancement of CO2 adsorption was propitious to the inhibition of carbon formation. The coke amount deposited on plasma treated catalyst was much smaller than that on the conventional catalyst.

  3. Air Oxidation of Activated Carbon to Synthesize a Biomimetic Catalyst for Hydrolysis of Cellulose.

    Science.gov (United States)

    Shrotri, Abhijit; Kobayashi, Hirokazu; Fukuoka, Atsushi

    2016-06-01

    Oxygenated carbon catalyzes the hydrolysis of cellulose present in lignocellulosic biomass by utilizing the weakly acidic functional groups on its surface. Here we report the synthesis of a biomimetic carbon catalyst by simple and economical air-oxidation of a commercially available activated carbon. Air- oxidation at 450-500 °C introduced 2000-2400 μmol g(-1) of oxygenated functional groups on the material with minor changes in the textural properties. Selectivity towards the formation of carboxylic groups on the catalyst surface increased with the increase in oxidation temperature. The degree of oxidation on carbon catalyst was found to be proportional to its activity for hydrolysis of cellulose. The hydrolysis of eucalyptus in the presence of carbon oxidized at 475 °C afforded glucose yield of 77 % and xylose yield of 67 %.

  4. Investigation of altenative carbon materials for fuel-cell catalyst support

    DEFF Research Database (Denmark)

    Larsen, Mikkel Juul

    In order to ensure high utilization of the catalyst material in a polymer electrolyte membrane fuel cell (PEMFC) it is usually fixed in the form of nanoparticles on a supporting material. The catalyst is platinum or a platinum alloy, and the commonly used support is carbon black (CB). Although...... the large surface area and good anchoring properties make it a suited material for this purpose, it is prone to degradation in the fuel-cell environment. Thus alternative materials with higher durability than CB, but with similar (or better) capability of dispersion, are desired. Among them are highly...... structured carbon forms such as graphitized CBs, carbon nanotubes (CNTs), and carbon nanofibres (CNFs). This thesis concerns the investigation of an array of different materials which may prospec-tively replace the conventional materials used in the catalyst. The study comprised 13 carbon samples which...

  5. Study on Diameter Controlled Growth of Carbon Nanotubes by LaAl1-xFexO3 Catalysts

    Institute of Scientific and Technical Information of China (English)

    PENG Feng; WANG Hong-juan

    2005-01-01

    A series of LaAl1-xFexO3 catalysts prepared with lanthanum nitrate, aluminium nitrate and iron nitrate was investigated in catalytical syntheses of carbon nanotubes with high yields and purity. The properties of carbon nanotubes prepared by the method of CVD(chemical vapor deposition) with n-hexane as the carbon resource were studied and it was shown that the diameter of carbon nanotubes can be controlled by the molar ratio of iron to aluminum in the catalysts and that the diameter of carbon nanotubes changes a little with the decrease of the iron content in the catalysts. From the TEM pictures of carbon nanotubes, it can be found that the LaAl1-xFexO3 catalysts have a significant influence on the wall thickness of the carbon nanotubes, whereas they have little influence on the inner diameter of the carbon nanotubes.

  6. Nickel catalysts for internal reforming in molten carbonate fuel cells

    NARCIS (Netherlands)

    Berger, R.J.; Doesburg, E.B.M.; Ommen, van J.G.; Ross, J.R.H.

    1996-01-01

    Natural gas may be used instead of hydrogen as fuel for the molten carbonate fuel cell (MCFC) by steam reforming the natural gas inside the MCFC, using a nickel catalyst (internal reforming). The severe conditions inside the MCFC, however, require that the catalyst has a very high stability. In orde

  7. Effect of Activated Carbon as a Support on Metal Dispersion and Activity of Ruthenium Catalyst for Ammonia Synthesis

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    Ten kinds of activated carbon from different raw materials were used as supports to prepare ruthenium catalysts. N2 physisorption and CO chemisorption were carried out to investigate the pore size distribution and the ruthenium dispersion of the catalysts. It was found that the Ru dispersion of the catalyst was closely related to not only the texture of carbon support but also the purity of activated carbon. The activities of a series of the carbon-supported barium-promoted Ru catalysts for ammonia synthesis were measured at 425 ℃, 10.0 MPa and 10 000 h-1. The result shows that the same raw material activated carbon, with a high purity, high surface area, large pore volume and reasonable pore size distribution might disperse ruthenium and promoter sufficiently, which activated carbon as support, could be used to manufacture ruthenium catalyst with a high activity for ammonia synthesis. The different raw material activated carbon as the support would greatly influence the catalytic properties of the ruthenium catalyst for ammonia synthesis. For example, with coconut shell carbon(AC1) as the support, the ammonia concentration in the effluent was 13.17% over 4%Ru-BaO/AC1 catalyst, while with the desulfurized coal carbon(AC10) as the support, that in the effluent was only 1.37% over 4%Ru-BaO/AC10 catalyst.

  8. Deactivation by carbon of iron catalysts for indirect liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Bartholomew, C.H.

    1991-01-10

    Although promoted cobalt and iron catalysts for Fischer-Tropsch (FT) synthesis of gasoline feedstock were first developed more than three decades ago, a major technical problem still limiting the commercial use of these catalysts today is carbon deactivation. This report describes recent progress in a fundamental, three-year investigation of carbon formation and its effects on the activity and selectivity of promoted iron catalysts for FT synthesis, the objectives of which are to: determine rates and mechanisms of carbon deactivation of unsupported Fe and Fe/K catalysts during CO hydrogenation over a range of CO concentrations, CO:H{sub 2} ratios, and temperatures; and model the rates of deactivation of the same catalysts in fixed-bed reactors. To accomplish the above objectives, the project is divided into the following tasks: (1) determine the kinetics of reaction and of carbon deactivation during CO hydrogenation on Fe and Fe/K catalysts coated on monolith bodies. (2) Determine the reactivities and types of carbon deposited during reaction on the same catalysts from temperature-programmed-surface-reaction spectroscopy (TPSR) and transmission electron microscopy (TEM). Determine the types of iron carbides formed at various temperatures and H{sub 2}/CO ratios using x-ray diffraction and Moessbauer spectroscopy. (3) Develop mathematical deactivation models which include heat and mass transport contributions for FT synthesis is packed-bed reactors. Progress to date is described. 48 refs., 3 figs., 1 tab.

  9. Synthesis, characterization and catalytic activity of carbon-silica hybrid catalyst from rice straw

    Science.gov (United States)

    Janaun, J.; Safie, N. N.; Siambun, N. J.

    2016-07-01

    The hybrid-carbon catalyst has been studied because of its promising potential to have high porosity and surface area to be used in biodiesel production. Silica has been used as the support to produce hybrid carbon catalyst due to its mesoporous structure and high surface area properties. The chemical synthesis of silica-carbon hybrid is expensive and involves more complicated preparation steps. The presence of natural silica in rice plants especially rice husk has received much attention in research because of the potential as a source for solid acid catalyst synthesis. But study on rice straw, which is available abundantly as agricultural waste is limited. In this study, rice straw undergone pyrolysis and functionalized using fuming sulphuric acid to anchor -SO3H groups. The presence of silica and the physiochemical properties of the catalyst produced were studied before and after sulphonation. The catalytic activity of hybrid carbon silica acid catalyst, (H-CSAC) in esterification of oleic acid with methanol was also studied. The results showed the presence of silica-carbon which had amorphous structure and highly porous. The carbon surface consisted of higher silica composition, had lower S element detected as compared to the surface that had high carbon content but lower silica composition. This was likely due to the fact that Si element which was bonded to oxygen was highly stable and unlikely to break the bond and react with -SO3H ions. H-CSAC conversions were 23.04 %, 35.52 % and 34.2 7% at 333.15 K, 343.15 K and 353.15 K, respectively. From this research, rice straw can be used as carbon precursor to produce hybrid carbon-silica catalyst and has shown catalytic activity in biodiesel production. Rate equation obtained is also presented.

  10. Carbon dioxide reforming of methane on monolithic Ni/Al2O3-based catalysts

    Institute of Scientific and Technical Information of China (English)

    S.O.Soloviev; A.Yu.Kapran; S.N.Orlyk; E.V.Gubareni

    2011-01-01

    Nickel-alumina catalysts supported on cordierite monoliths of honeycomb structure surpass essentially the conventional granulated ones with respect to the output in carbon dioxide reforming of methane.Adjusting the surface acid-base properties of catalysts by introduction of alkali metal(Na,K)oxides inhibits the carbonization and as a result,improves the operational stability of these catalysts.An effect of promotion of nickel-alumina based composite doped by lanthanum oxide is found.This effect,caused by an additional route for the CO2 activation on Ni-La2O3/Al2O3/cordierite catalyst,is displayed in increase of methane conversion under conditions of an oxidant excess.

  11. Effects of bimetallic catalysts on synthesis of nitrogen-doped carbon nanotubes as nanoscale energetic materials

    Institute of Scientific and Technical Information of China (English)

    Hao Liu; Yong Zhang; Ruying Li; Xueliang Sun; Hakima Abou-Rachid

    2011-01-01

    Well aligned nitrogen-doped carbon nanotubes (CNx-NTs),as energetic materials,are synthesized on a silicon substrate by aerosol-assisted chemical vapor deposition.Tungsten (W) and molybdenum (Mo) metals are respectively introduced to combine with iron (Fe) to act as a bimetallic co-catalyst layer.Correlations between the composition and shape of the co-catalyst and morphology,size,growth rate and nitrogen doping amount of the synthesized CNx-NTs are investigated by secondary and backscattered electron imaging in a field emission scanning electron microscope (FESEM) and X-ray photoelectron spectrometer (XPS).Compared to pure iron catalyst.W-Fe co-catalyst can result in lower growth rate,larger diameter and wider size distribution of the CNx-NTs; while incorporation of molybdenum into the iron catalyst layer can reduce the diameter and size distribution of the nanotubes.Compared to the sole iron catalyst,Fe-W catalyst impedes nitrogen doping while Fe-Mo catalyst promotes the incorporation of nitrogen into the nanotubes.The present work indicates that CNx-NTs with modulated size,growth rate and nitrogen doping concentration are expected to be synthesized by tuning the size and composition of co-catalysts,which may find great potential in producing CNx-NTs with controlled structure and properties.

  12. Preparation of arrays of long carbon nanotubes using catalyst structure

    Energy Technology Data Exchange (ETDEWEB)

    Zhu, Yuntian T.; Arendt, Paul; Li, Qingwen; Zhang, Xiefie

    2016-03-22

    A structure for preparing an substantially aligned array of carbon nanotubes include a substrate having a first side and a second side, a buffer layer on the first side of the substrate, a catalyst on the buffer layer, and a plurality of channels through the structure for allowing a gaseous carbon source to enter the substrate at the second side and flow through the structure to the catalyst. After preparing the array, a fiber of carbon nanotubes may be spun from the array. Prior to spinning, the array can be immersed in a polymer solution. After spinning, the polymer can be cured.

  13. Support effect on carbon nanotube growth by methane chemical vapor deposition on cobalt catalysts

    International Nuclear Information System (INIS)

    The influence of the support on carbon nanotube production by methane chemical vapor deposition (CVD) on cobalt catalysts was investigated. N2 physisorption, X-ray diffractometry (XRD), temperature programmed reduction (TPR) and H2 and CO chemisorption techniques were used to characterize the structure of cobalt catalysts supported on different metal oxides (Al2O3, SiO2, Nb2O5 and TiO2). Raman spectroscopy, temperature programmed oxidation (TPO) and scanning electron microscopy (SEM) were used for the characterization and quantification of produced carbon species. On carbon nanotube growth, the catalyst produced three main carbon species: amorphous carbon, single walled carbon nanotubes (SWNT) and multi walled carbon nanotubes (MWNT). The characterization techniques showed that the catalyst selectivity to each kind of nanotube depended on the cobalt particle size distribution, which was influenced by the textural properties of the support. Co/TiO2 showed the highest selectivity towards single wall nanotube formation. This high selectivity results from the narrow size distribution of cobalt particles on TiO2. (author)

  14. Carbon dioxide as a carbon source in organic transformation: carbon-carbon bond forming reactions by transition-metal catalysts.

    OpenAIRE

    Tsuji, Yasushi; Fujihara, Tetsuaki

    2012-01-01

    Recent carbon-carbon bond forming reactions of carbon dioxide with alkenes, alkynes, dienes, aryl zinc compounds, aryl boronic esters, aryl halides, and arenes having acidic C-H bonds are reviewed in which transition-metal catalysts play an important role.

  15. Methanol dehydration on carbon-based acid catalysts

    OpenAIRE

    Valero-Romero, Mª José; Calvo-Muñoz, Elisa Mª; Ruiz-Rosas, Ramiro; Rodríguez-Mirasol, José; Cordero, Tomás

    2013-01-01

    Methanol dehydration to produce dimethyl ether (DME) is an interesting process for the chemical industry since DME is an important intermediate and a promising clean alternative fuel for diesel engines. Pure or modified γ-aluminas (γ-Al2O3) and zeolites are often used as catalysts for this reaction. However, these materials usually yield non desirable hydrocarbons and undergo fast deactivation. In this work, we study the catalytic conversion of methanol over an acid carbon catalyst obtaine...

  16. Chlorination of Carbon Nanotubes Obtained on the Different Metal Catalysts

    Directory of Open Access Journals (Sweden)

    Iwona Pełech

    2013-01-01

    Full Text Available In this paper, a chlorination method is proposed for simultaneous purification and functionalization of carbon nanotubes, thus increasing their ability to use. Carbon nanotubes were obtained by CVD method through ethylene decomposition on the nanocrystalline iron or cobalt or bimetallic iron-cobalt catalysts. The effects of temperature (50, 250, and 450°C in the case of carbon nanotubes obtained on the Fe-Co catalyst and type of catalyst (Fe, Co, Fe/Co on the effectiveness of the treatment and functionalization were tested. The phase composition of the samples was determined using the X-ray diffraction method. The quantitative analysis of metal impurity content was validated by means of the thermogravimetric analysis. Using X-ray Photoelectron Spectroscopy (XPS, Energy Dispersive Spectroscopy (EDS analysis, and also Mohr titration method, the presence of chlorine species on the surface of chlorinated samples was confirmed.

  17. Graphitised Carbon Nanofibres as Catalyst Support for PEMFC

    DEFF Research Database (Denmark)

    Yli-Rantala, E.; Pasanen, A.; Kauranen, P.;

    2011-01-01

    Graphitised carbon nanofibres (G-CNFs) show superior thermal stability and corrosion resistance in PEM fuel cell environment over traditional carbon black (CB) and carbon nanotube catalyst supports. However, G-CNFs have an inert surface with only very limited amount of surface defects for the anc......Graphitised carbon nanofibres (G-CNFs) show superior thermal stability and corrosion resistance in PEM fuel cell environment over traditional carbon black (CB) and carbon nanotube catalyst supports. However, G-CNFs have an inert surface with only very limited amount of surface defects...... for the anchorage of Pt catalyst nanoparticles. Modification of the fibre surface is therefore needed. In this study Pt nanoparticles have been deposited onto as-received and surface-modified G-CNFs. The surface modifications of the fibres comprise acid treatment and nitrogen doping by pyrolysis of a polyaniline...... (PANI) precursor. The modified surfaces were studied by FTIR and XPS and the electrochemical characterization, including long-term Pt stability tests, was performed using a low-temperature PEMFC single cell. The performance and stability of the G-CNF supported catalysts were compared with a CB supported...

  18. New efficient catalyst for ammonia synthesis: barium-promoted cobalt on carbon

    DEFF Research Database (Denmark)

    Hagen, Stefan; Barfod, Rasmus; Fehrmann, Rasmus;

    2002-01-01

    Barium-promoted cobalt catalysts supported on carbon exhibit higher ammonia activities at synthesis temperatures than the commercial, multipromoted iron catalyst and also a lower ammonia......Barium-promoted cobalt catalysts supported on carbon exhibit higher ammonia activities at synthesis temperatures than the commercial, multipromoted iron catalyst and also a lower ammonia...

  19. Nanoscaled palladium catalysts on activated carbon support "Sibunit" for fine organic synthesis

    Science.gov (United States)

    Simakova, I.; Koskin, A.; Deliy, I.; Simakov, A.

    2005-08-01

    The application of nanosized palladium catalysts has gained growing importance over the last few years. Palladiumbased catalytic methods for fine organic synthesis permits the replacement of traditional labor-consuming techniques in multi-step organic syntheses and provides an improvement from the standpoint of cost and environmental impact. The use of activated carbon "Sibunit" as a substrate for catalysts has been fostered by the substrate's high surface area, chemical inertness both in acidic and basic media, and at the same time by the absence of very strong acidic centers on its surface which could promote undesirable side reactions during the catalytic run. A conversion of alpha-pinene derivatives to commercial biologically active compounds and fragrances as well as sun screens with ultra violet filtering properties, involves a catalytic hydrogenation as a key intermediate step. The aim of the present work is to clarify the factors favoring the dispersion of Pd metal on carbon. The effect of reduction temperature and pretreatment of the carbon surface on metal size during preparation of Pd on "Sibunit" catalysts for selective verbenol conversion was studied. The electron microscopy method (TEM) was used to show the influence on Pd metal dispersion of carbon surface oxidation by the oxidant H2O2, HNO3. The catalytic activity of Pd/C catalyst samples in verbenol hydrogenation reaction was determined. Kinetic peculiarities of verbenol hydrogenation over the most active catalyst sample were obtained.

  20. Catalyst deposition for the preparation of carbon nanotubes

    DEFF Research Database (Denmark)

    2013-01-01

    Disclosed is a method of depositing islands of catalyst with a predetermined density, wherein in said method comprises the steps of: obtaining a diffusion barrier covered nano patterned surface comprising a plurality of plateaus, having a density of plateaus dependent on the predetermined density...... patterned surface is configured to ensure that no more than a single island of catalyst is formed on each plateau, so that a sub sequent growth of carbon nanotubes from the deposited islands result in that no more than a single carbon nanotube is grown from each plateau....

  1. Catalyst Deactivation Simulation Through Carbon Deposition in Carbon Dioxide Reforming over Ni/CaO-Al2O3 Catalyst

    Directory of Open Access Journals (Sweden)

    Istadi Istadi

    2011-11-01

    Full Text Available Major problem in CO2 reforming of methane (CORM process is coke formation which is a carbonaceous residue that can physically cover active sites of a catalyst surface and leads to catalyst deactivation. A key to develop a more coke-resistant catalyst lies in a better understanding of the methane reforming mechanism at a molecular level. Therefore, this paper is aimed to simulate a micro-kinetic approach in order to calculate coking rate in CORM reaction. Rates of encapsulating and filamentous carbon formation are also included. The simulation results show that the studied catalyst has a high activity, and the rate of carbon formation is relatively low. This micro-kinetic modeling approach can be used as a tool to better understand the catalyst deactivation phenomena in reaction via carbon deposition. Copyright © 2011 BCREC UNDIP. All rights reserved.(Received: 10th May 2011; Revised: 16th August 2011; Accepted: 27th August 2011[How to Cite: I. Istadi, D.D. Anggoro, N.A.S. Amin, and D.H.W. Ling. (2011. Catalyst Deactivation Simulation Through Carbon Deposition in Carbon Dioxide Reforming over Ni/CaO-Al2O3 Catalyst. Bulletin of Chemical Reaction Engineering & Catalysis, 6 (2: 129-136. doi:10.9767/bcrec.6.2.1213.129-136][How to Link / DOI: http://dx.doi.org/10.9767/bcrec.6.2.1213.129-136 || or local:  http://ejournal.undip.ac.id/index.php/bcrec/article/view/1213 ] | View in  |  

  2. Activated Carbon, Carbon Nanofiber and Carbon Nanotube Supported Molybdenum Carbide Catalysts for the Hydrodeoxygenation of Guaiacol

    Directory of Open Access Journals (Sweden)

    Eduardo Santillan-Jimenez

    2015-03-01

    Full Text Available Molybdenum carbide was supported on three types of carbon support—activated carbon; multi-walled carbon nanotubes; and carbon nanofibers—using ammonium molybdate and molybdic acid as Mo precursors. The use of activated carbon as support afforded an X-ray amorphous Mo phase, whereas crystalline molybdenum carbide phases were obtained on carbon nanofibers and, in some cases, on carbon nanotubes. When the resulting catalysts were tested in the hydrodeoxygenation (HDO of guaiacol in dodecane, catechol and phenol were obtained as the main products, although in some instances significant amounts of cyclohexane were produced. The observation of catechol in all reaction mixtures suggests that guaiacol was converted into phenol via sequential demethylation and HDO, although the simultaneous occurrence of a direct demethoxylation pathway cannot be discounted. Catalysts based on carbon nanofibers generally afforded the highest yields of phenol; notably, the only crystalline phase detected in these samples was Mo2C or Mo2C-ζ, suggesting that crystalline Mo2C is particularly selective to phenol. At 350 °C, carbon nanofiber supported Mo2C afforded near quantitative guaiacol conversion, the selectivity to phenol approaching 50%. When guaiacol HDO was performed in the presence of acetic acid and furfural, guaiacol conversion decreased, although the selectivity to both catechol and phenol was increased.

  3. Magnetic Carbon Supported Palladium Nanoparticles: An Efficient and Sustainable Catalyst for Hydrogenation Reactions

    Science.gov (United States)

    Magnetic carbon supported Pd catalyst has been synthesized via in situ generation of nanoferrites and incorporation of carbon from renewable cellulose via calcination; the catalyst can be used for the hydrogenation of alkenes and reduction of aryl nitro compounds.

  4. Deactivation by carbon of iron catalysts for indirect liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Bartholomew, C H

    1991-02-14

    Progress is reported for a four-year fundamental investigation of carbon formation and its effects on the activity and selectivity of promoted iron catalysts for FT synthesis, the objectives of which were to (1) determine rates and mechanisms of carbon deactivation of unsupported Fe and Fe/K catalysts during CO hydrogenation and (2) model the global rates of deactivation at the surface of the catalyst for the same catalysts. A computer-automated reactor system to be used in the kinetic and deactivation studies was designed, constructed and tested. Kinetic data for CO hydrogenation on unsupported, unpromoted iron, 99% Fe/1% Al{sub 2}O{sub 3}, and K-promoted 99% Fe/1% Al{sub 2}O{sub 3} catalysts were obtained as functions of temperature, reactant particle pressures and time. The activity/selectivity and kinetic data are consistent with those previously reported for supported, unpromoted and promoted iron. Two kinds of deactivation were observed during FT synthesis on these samples: (1) loss of surface area after reduction of unsupported, unpromoted iron at 400{degree}C and (2) loss of activity with time due to carbon deposition, especially in the case of K-promoted 99% Fe/1% A1{sub 2}O{sub 3}. Deactivation rate data were obtained for CO hydrogenation on promoted Fe as a function of time, temperature, and H{sub 2}/CO ratio. 50 refs., 24 figs., 5 tabs.

  5. Thermally Activated Palm Kernel Based Carbon as a Support for Edible Oil Hydrogenation Catalyst

    Directory of Open Access Journals (Sweden)

    Abdulmajid Alshaibani

    2013-01-01

    Full Text Available Activated carbon has distinctive properties as a support for hydrogenation catalysts. Thermally activated carbon has been prepared from palm kernel shell at 1073 K and placed under nitrogen flow for 2 h. It was impregnated by palladium using toluene solution of Pd (acac2. The Pd/C was reduced using a water solution of potassium borohydride (KBH4. The Pd-B/C was characterized by the Brunauer-Emmett-Teller surface area analysis (BET, scanning electron microscopy (SEM, transmission electron microscopy (TEM and inductively-coupled plasma mass spectrometry (ICP-MS. Pd-B/C was applied for sunflower oil hydrogenation at a temperature of 373 K, hydrogen pressure of 413.5 kPa and agitation of 1400 rpm for 1 h. Pd-B/C noticeably exhibited a higher overall catalyst activity in comparison to some recently published palladium catalysts.

  6. Deactivation by carbon of iron catalysts for indirect liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Bartholomew, C.H.

    1990-10-29

    This report describes recent progress in a fundamental, three-year investigation of carbon formation and its effects on the activity and selectivity of promoted iron catalysts for synthesis, the objectives of which are: determine rates and mechanisms of carbon deactivation of unsupported Fe and Fe/K catalysts during CO hydrogenation over a range of CO concentrations, CO:H{sub 2} ratios, and temperatures; model the rates of deactivation of the same catalysts in fixed-bed reactors. During the fourteenth quarter design of software for a computer-automated reactor system to be used in the kinetic and deactivation studies was continued. Further progress was made toward the completion of the control language, control routines, and software for operating this system. Progress was also made towards testing of the system hardware and software. 47 refs.

  7. Novel Ru - K/Carbon Nanotubes Catalyst for Ammonia Synthesis

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    A novel ammonia synthesis catalyst, potassium-promoted ruthenium supported on carbon nanotubes, was developed. It was found that the Ru-K/carbon nanotubes catalyst had higher activity for ammonia synthesis ( 20.85 ml NH 3 /h/g-cat ) than the Ru-K/fullerenes ( 13.3 ml NH 3 /h/g-cat ) at atmospheric ressure and 623 K. The catalyst had activity even at 473 K, and had the highest activity ( 23.46 ml NH 3 /h/g-cat ) at 643 K. It was suggested that the multi-walled structure favored the electron transfer, the hydrogen-storage and the hydrogen-spill which were favorable to ammonia synthesis.

  8. Carbon Nanotubes Synthesis via Arc Discharge with a Yttria Catalyst

    OpenAIRE

    M. I. Mohammad; Ahmed A. Moosa; J.H. Potgieter; Mustafa K. Ismael

    2013-01-01

    A facile method is proposed to use a computer controlled Arc discharge gap between graphite electrodes together with an yttria-nickel catalyst to synthesize carbon nanotubes under an Ar-H2 gases mixture atmosphere by applying different DC currents and pressure. This produces carbon nanotubes with decreased diameters and increased length. XRD evidence indicated a shift toward higher crystallinity nanotubes. Yields of the CNTs after purification were also enhanced.

  9. Investigation of the electrospun carbon web as the catalyst layer for vanadium redox flow battery

    Science.gov (United States)

    Wei, Guanjie; Fan, Xinzhuang; Liu, Jianguo; Yan, Chuanwei

    2014-12-01

    Polyacrylonitrile (PAN) carbon nonwoven web consisting of 100-200 nm ultrafine fibers has been developed by electrospinning and subsequent carbonization process at 1000 °C for different times. The surface morphology, composition, structure, and electrical conductivity of the electrospun carbon webs (ECWs) as well as their electrochemical properties toward vanadium redox couples have been characterized. With the increasing of carbonization time, the electrochemical reversibility of the vanadium redox couples on the ECW is enhanced greatly. As the carbonization time increases up to 120 min, the hydrogen evolution is facilitated while the reversibility is promoted a little bit further. The excellent performance of ECW may be attributed to the conversion of fibers carbon structure and improvement of electrical conductivity. Due to the good electrochemical activity and freestanding 3-dimensional structure, the ECW carbonized for 90 min is used as catalyst layer in vanadium redox flow battery (VRFB) and enhances the cell performance.

  10. Pt/Al/sub 2/O/sub 3/- carbon nanocomposite as a catalyst for fuel cells

    International Nuclear Information System (INIS)

    Catalysts comprising platinum nanoparticles (Pt NPs) on carbon support are used in fuel cells for the hydrogen and electricity production by electrochemical oxidation of methanol. However, the catalyst is not the best in terms of its performance. Considering role of the support as significant towards efficiency and durability of the catalyst, there is need for introducing novel support materials to replace carbon alone. Deposition of various metallic NPs on ceramic-carbon (hybrid) supports has been reported to improve thermal, mechanical, electrical and chemical properties of different types of catalyst. In search of better performing catalysts for proton exchange membrane fuel cells (PEMFCs), hybrid supports having different ceramic materials should be synthesized. In this regard Pt/Al/sub 2/O/sub 3/-Carbon (nanocomposites) have been synthesized and applied as promising catalysts in the PEMFCs; results obtained for the nanocomposites were compared with Pt/carbon and Pt/Al/sub 2/O/sub 3/. Vulcan carbon was purified and functionalized prior to use; presence of oxygen containing functional groups on carbon was established from the FTIR spectrum, Hybrid support (1:8 by weight ratio of ceramic and carbon) were already prepared in aqueous 2-propanol employing sonication method on to which Pt NPs (10% by weight in all the cases) were deposited by simple chemical reduction of PtCl/sub 4/ by NaBH/sub 4/ under controlled conditions. The catalysts were subjected to various characterization techniques like TGA (for thermal stability), EDX (for chemical composition), SEM (for surface morphology) and XRD (for cell-shape and -volume, material density and average crystalline size). Catalysts efficiencies for the methanol oxidation were investigated through cyclic voltammetery (CV) by comparing electrochemical surface area, peak current, exchange current density and rate constant in the acidic and basic media. Pt/Al/sub 2/O/sub 3/-carbon exhibited better catalytic efficiencies

  11. Carbon Nanotubes Supported Pt-Ru-Ni as Methanol Electro-Oxidation Catalyst for Direct Methanol Fuel Cells

    Institute of Scientific and Technical Information of China (English)

    Fei Ye; Shengzhou Chen; Xinfa Dong; Weiming Lin

    2007-01-01

    Carbon nanotubes (CNTs) supported Pt-Ru and Pt-Ru-Ni catalysts were prepared by chemical reduction of metal precursors with sodium borohydride at room temperature. The crystallographic properties and composition of the catalysts were characterized by X-ray diffraction (XRD) and energy dispersive X-ray (EDX) analysis, and the catalytic activity and stability for methanol electro-oxidation were measured by electrochemical impedance spectroscopy (EIS), linear sweep voltammetries (LSV), and chronoamperometry (CA). The results show that the catalysts exhibit face-centered cubic (fcc) structure.The particle size of Pt-Ru-Ni/CNTs catalyst is about 4.8 nm. The catalytic activity and stability of the Pt-Ru-Ni/CNTs catalyst are higher than those of Pt-Ru/CNTs catalyst.

  12. Understanding properties of engineered catalyst supports using contact angle measurements and X-ray reflectivity.

    Science.gov (United States)

    Amama, Placidus B; Islam, Ahmad E; Saber, Sammy M; Huffman, Daniel R; Maruyama, Benji

    2016-02-01

    There is significant interest in broadening the type of catalyst substrates that support the growth of high-quality carbon nanotube (CNT) carpets. In this study, ion beam bombardment has been utilized to modify catalyst substrates for CNT carpet growth. Using a combination of contact angle measurements (CAMs) and X-ray reflectivity (XRR) for the first time, new correlations between the physicochemical properties of pristine and engineered catalyst substrates and CNT growth behavior have been established. The engineered surfaces obtained after exposure to different degrees of ion beam damage have distinct physicochemical properties (porosity, layer thickness, and acid-base properties). The CAM data were analyzed using the van Oss-Chaudhury-Good model, enabling the determination of the acid-base properties of the substrate surfaces. For the XRR data, a Fourier analysis of the interference patterns enabled extraction of layer thickness, while the atomic density and interfacial roughness were extracted by analyzing the amplitude of the interference oscillations. The dramatic transformation of the substrate from "inactive" to "active" is attributed to a combined effect of substrate porosity or damage depth and Lewis basicity. The results reveal that the efficiency of catalyst substrates can be further improved by increasing the substrate basicity, if the minimum surface porosity is established. This study advances the use of a non-thermochemical approach for catalyst substrate engineering, as well as demonstrates the combined utility of CAM and XRR as a powerful, nondestructive, and reliable tool for rational catalyst design.

  13. VPO catalysts synthesized on substrates with modified activated carbons

    International Nuclear Information System (INIS)

    VPO catalysts were prepared on oxidized and unoxidized activated carbons differing in initial porous structure. Carbons were oxidized under relatively soft (30% H2O2, 200 deg. C) and hard (50% H2O2, 350 deg. C) conditions. Carbon modification was carried out hydrothermally in a traditional autoclave (HTT) or a microwave reactor (MWT). The synthesis was also carried out under hydrothermal (HTS or MWS) conditions. V2O5 and NH4VO3 were used as precursors. The samples are characterized by diversified porous structure at SBET = 732-1617 m2/g and Vpor = 0.44-0.90 cm3/g, as well as various degree of VPO crystallinity. Possibility of preparation of the VPO catalysts under ecologically appropriate conditions, i.e. in aqueous solutions, was shown.

  14. Effect of the ruthenium loading and barium addition on the activity of ruthenium/carbon catalysts in carbon monoxide methanation

    Directory of Open Access Journals (Sweden)

    Truszkiewicz Elżbieta

    2014-12-01

    Full Text Available A group of supported ruthenium catalysts was prepared and tested in methanation of small CO amounts (7000 ppm in hydrogen-rich streams. High surface area graphitized carbon (484 m2/g was used as a support for ruthenium and RuCl3 was used as a Ru precursor. Some of the Ru/C systems were additionally doped with barium (Ba(NO32 was barium precursor. The catalysts were characterized by the chemisorption technique using CO as an adsorbate. To determine the resistance of the catalysts to undesired carbon support methanation, the TG-MS experiments were performed. They revealed that the barium addition inhibits support losses. The studies of CO methanation (fl ow reactor, atmospheric pressure have shown that some of the supported ruthenium catalysts exhibit high activities referred to the metal mass. The catalytic properties of ruthenium proved to be dependent on metal dispersion. Some of the Ru/C and Ba-Ru/C systems exhibit higher activity in CO hydrogenation than the commercial nickel-based catalyst.

  15. Methane Decomposition into Carbon Fibers over Coprecipitated Nickel-Based Catalysts

    Institute of Scientific and Technical Information of China (English)

    Yan Ju; Fengyi Li; Renzhong Wei

    2005-01-01

    Decomposition of methane in the presence of coprecipitated nickel-based catalysts to produce carbon fibers was investigated. The reaction was studied in the temperature range of 773 K to 1073 K.At 1023 K, the catalytic activities of three catalysts kept high at the initial period and then decreased with the reaction time. The lifetimes of Ni-Cu-Al and Ni-La-Al catalysts are longer than that of Ni-Al catalyst. With three catalysts, the yield of carbon fibers was very low at 773 K. The yield of carbon fibers for Ni-La-Al catalyst was more than those for Ni-Al and Ni-Cu-Al catalysts. For Ni-La-Al catalyst, the elevation of temperature from 873 K up to 1073 K led gradually to an increase in the yield of carbon fibers.XRD studies on the Ni-La-Al catalyst indicate that La2NiO4 was formed. The formation of La2NiO4 is responsible for the increase in the catalytic lifetime and the yield of carbon fibers synthesized on Ni-La-Al at 773-1073 K. Carbon fibers synthesized on Ni-Al catalyst are thin, long carbon nanotubes. There are bamboo-shaped carbon fibers synthesized on Ni-Cu-Al catalyst. Carbon fibers synthesized on Ni-La-Al catalyst have large hollow core, thin wall and good graphitization.

  16. Nickel catalysts supported on MgO with different specific surface area for carbon dioxide reforming of methane

    Institute of Scientific and Technical Information of China (English)

    Luming; Zhang; Lin; Li; Yuhua; Zhang; Yanxi; Zhao; Jinlin; Li

    2014-01-01

    In this paper, three kinds of MgO with different specific surface area were prepared, and their effects on the catalytic performance of nickel catalysts for the carbon dioxide reforming of methane were investigated. The results showed that MgO support with the higher specific surface area led to the higher dispersion of the active metal, which resulted in the higher initial activity. On the other hand, the specific surface area of MgO materials might not be the dominant factor for the basicity of support to chemisorb and activate CO2, which was another important factor for the performance of catalysts. Herein, Ni/MgO(CA) catalyst with proper specific surface area and strong ability to activate CO2exhibited stable catalytic property and the carbon species deposited on the Ni/MgO(CA) catalyst after 10 h of reaction at 650 ?C were mainly activated carbon species.

  17. Structure and properties of carbon nanofibers. application as electrocatalyst support

    Directory of Open Access Journals (Sweden)

    S. del Rio

    2012-03-01

    Full Text Available The present work aimed to gain an insight into the physical-chemical properties of carbon nanofibers and the relationship between those properties and the electrocatalytic behavior when used as catalyst support for their application in fuel cells.

  18. Characterization of a surface modified carbon cryogel and a carbon supported Pt catalyst

    Directory of Open Access Journals (Sweden)

    BILJANA M. BABIĆ

    2007-08-01

    Full Text Available A carbon cryogel, synthesized by carbonization of a resorcinol/formaldehyde cryogel and oxidized in nitric acid, was used as catalyst support for Pt nano-particles. The Pt/C catalyst was prepared by a modified polyol synthesis method in an ethylene glycol (EG solution. Characterization by nitrogen adsorption showed that the carbon cryogel support and the Pt/C catalyst were mesoporous materials with high specific surface areas (SBET > 400 m2 g-1 and large mesoporous volumes. X-Ray diffraction of the catalyst demonstrated the successful reduction of the Pt precursor to metallic form. TEM Images of the Pt/C catalyst and Pt particle size distribution showed that the mean Pt particle size was about 3.3 nm. Cyclic voltammetry (CV experiments at various scan rates (from 2 to 200 mV s-1 were performed in 0.5 mol dm-3 HClO4 solution. The large capacitance of the oxidized carbon cryogel electrode, which arises from a combination of the double-layer capacitance and pseudocapacitance, associated with the participation of surface redox-type reactions was demonstrated. For the oxidized carbon cryogel, the total specific capacitance determined by 1/C vs. ν0.5 extrapolation method was found to be 386 F g-1. The hydrogen oxidation reaction at the investigated Pt/C catalyst proceeded as an electrochemically reversible, two-electron direct discharge reaction.

  19. Synthesis and Growth Mechanism of Carbon Filaments by Chemical Vapor Deposition without Catalyst

    Institute of Scientific and Technical Information of China (English)

    Shuhe Liu; Feng Li; Shuo Bai

    2009-01-01

    Carbon filaments with diameter from several to hundreds micrometers were synthesized by chemical vapor deposition of methane without catalyst. The morphology, microstructure and mechanical properties of the carbon filament were investigated by scanning electronic microscopy, optical microscopy, X-ray diffraction and mechanical testing. The results show that the carbon filament is inverted cone shape and grows up along the gas flow direction. The stem of it is formed of annular carbon layers arranged in a tree ring structure while the head is made up of concentrical layers. The tensile strength of the carbon filament is increased after graphitization for the restructuring and growing large of graphene. The growth mechanism of carbon filament was proposed according to the results of two series of experiments with different deposition time and intermittent deposition cycles.

  20. Deactivation by carbon of iron catalysts for indirect liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Bartholomew, C.H.

    1990-10-11

    This report describes recent progress in a fundamental, three-year investigation of carbon formation and its effects on the activity and selectivity of promoted iron catalysts for Fischer-Tropsch (FT) synthesis, the objectives of which are: determine rates and mechanisms of carbon deactivation of unsupported Fe and Fe/K catalysts during CO hydrogenation over a range of CO concentrations, CO:H{sub 2} ratios, and temperatures; model the rates of deactivation of the same catalysts in fixed-bed reactors. During the thirteenth quarter design of software for a computer-automated reactor system to be used in the kinetic and deactivation studies was continued. Further progress was made toward the completion of the control language, control routines, and software for operating this system. Progress was also made on the testing of the system hardware and software. H{sub 2} chemisorption capacities and activity selectivity data were also measured for three iron catalysts promoted with 1% alumina. 47 refs., 8 figs., 1 tab.

  1. Properties of the FCC Catalyst Additive Prepared from Guizhou Kaoline

    Directory of Open Access Journals (Sweden)

    Xianlun Xu

    2006-09-01

    Full Text Available The properties of a FCC catalyst additive prepared from Guizhou kaoline were extensively investigated. The samples were characterized by N2 adsorption, X-ray diffraction, IR spectrometry, and scanning electron microscope (SEM. The results showed that the crystallinity of NaY zeolite synthesized from this kaoline was 25% and the silica alumina ratio was rk/s ˇ m = 5.05. The catalyst additive prepared from above crystallization product exhibited excellent performance of nickel and vanadium passivation, offered 21% lower coke versus base catalyst, while maintaining high bottoms upgrading selectivity.

  2. Sustainable catalyst supports for carbon dioxide gas adsorbent

    Science.gov (United States)

    Mazlee, M. N.

    2016-07-01

    The adsorption of carbon dioxide (CO2) become the prime attention nowadays due to the fact that increasing CO2 emissions has been identified as a contributor to global climate change. Major sources of CO2 emissions are thermoelectric power plants and industrial plants which account for approximately 45% of global CO2 emissions. Therefore, it is an urgent need to develop an efficient CO2 reduction technology such as carbon capture and storage (CCS) that can reduce CO2 emissions particularly from the energy sector. A lot of sustainable catalyst supports have been developed particularly for CO2 gas adsorbent applications.

  3. Surface chemistry of metal catalyst under carbon nanotube growth conditions

    Science.gov (United States)

    Back, Tyson Cody

    The catalyst nanoparticle is critical to the yield, type, and diameter in the growth and nucleation of carbon nanotubes. The objective of this study is focused on determining what changes take place with the catalyst chemistry under growth conditions typically seen in chemical vapor deposition, CVD, experiments. It is well known that catalyst poisoning can occur and in turn effects the catalytic activity of the nanoparticle. A complete description of this mechanism is as of yet undetermined. In order to elucidate this process iron films were deposited onto Si substrates that contained a support layer of Al2O3 or SiO2. These samples were investigated with various surface chemistry techniques such as X-ray photoelectron spectroscopy (XPS), Auger electron spectroscopy (AES), and electron energy loss spectroscopy (EELS). In addition, structural characteristics were investigated with scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The surface techniques were used in-situ in order to observe chemistries that might not be observable outside a CVD reactor. Two sets of experiments were performed on the silica and alumina supports. The first consisted of carbon nanotube growth at near atmospheric pressure, while the second was performed under vacuum. The oxide support was shown to have an affect on the type of nanotubes grown under identical conditions. The silica support films produced more MWNT, while the alumina support films produced more SWNT. This difference was due to the amount of ripening that takes place on the oxide supports. Also in-situ XPS revealed differences in the chemistry of iron catalyst during growth and these differences were attributed to substrate interactions between alumina and iron. Finally, in-situ XPS analysis showed no evidence of carbides or oxides acting as a catalyst during the nucleation process.

  4. High performance low temperature carbon composite catalysts for flexible dye sensitized solar cells.

    Science.gov (United States)

    Hashmi, Syed Ghufran; Halme, Janne; Saukkonen, Tapio; Rautama, Eeva-Leena; Lund, Peter

    2013-10-28

    Roll-to-roll manufacturing of dye sensitized solar cells (DSSCs) requires efficient and low cost materials that adhere well on the flexible substrates used. In this regard, different low temperature carbon composite counter electrode (CE) catalyst ink formulations for flexible DSSCs were developed that can be simply and quickly coated on plastic substrates and dried below 150 °C. The CEs were investigated in terms of photovoltaic performance in DSSCs by current-voltage measurements, mechanical adhesion properties by bending and tape tests, electro-catalytic performance by electrochemical impedance spectroscopy and microstructure by electron microscopy. In the bending and tape tests, PEDOT-carbon composite catalyst layers exhibited higher elasticity and better adhesion on all the studied substrates (ITO-PET and ITO-PEN plastic, and FTO-glass), compared to a binder free carbon composite and a TiO2 binder enriched carbon composite, and showed lower charge transfer resistance (1.5-3 Ω cm(2)) than the traditional thermally platinized CE (5 Ω cm(2)), demonstrating better catalytic performance for the tri-iodide reduction reaction. Also the TiO2 binder enriched carbon composite showed good catalytic characteristics and relatively good adhesion on ITO-PET, but on ITO-PEN its adhesion was poor. A DSSC with the TiO2 binder enriched catalyst layer reached 85% of the solar energy conversion efficiency of the reference DSSC based on the traditional thermally platinized CE. Based on the aforementioned characteristics, these carbon composites are promising candidates for replacing the platinum catalyst in a high volume roll-to-roll manufacturing process of DSSCs. PMID:24042582

  5. Hydrogen Production by Steam Reforming of Liquefied Natural Gas (LNG) Over Nickel-Phosphorus-Alumina Xerogel Catalyst Prepared by a Carbon-Templating Epoxide-Driven Sol-Gel Method.

    Science.gov (United States)

    Bang, Yongju; Park, Seungwon; Han, Seung Ju; Yoo, Jaekyeong; Choi, Jung Ho; Kang, Tae Hun; Lee, Jinwon; Song, In Kyu

    2016-05-01

    A nickel-phosphorus-alumina xerogel catalyst was prepared by a carbon-templating epoxide-driven sol-gel method (denoted as CNPA catalyst), and it was applied to the hydrogen production by steam reforming of liquefied natural gas (LNG). For comparison, a nickel-phosphorus-alumina xerogel catalyst was also prepared by a similar method in the absence of carbon template (denoted as NPA catalyst). The effect of carbon template addition on the physicochemical properties and catalytic activities of the catalysts in the steam reforming of LNG was investigated. Both CNPA and NPA catalysts showed excellent textural properties with well-developed mesoporous structure. However, CNPA catalyst retained a more reducible nickel aluminate phase than NPA catalyst. XRD analysis of the reduced CNPA and NPA catalysts revealed that nickel sintering on the CNPA catalyst was suppressed compared to that on the NPA catalyst. From H2-TPD and CH4-TPD measurements of the reduced CNPA and NPA catalysts, it was also revealed that CNPA catalyst with large amount of hydrogen uptake and strong hydrogen-binding sites showed larger amount of methane adsorption than NPA catalyst. In the hydrogen production by steam reforming of LNG, CNPA catalyst with large methane adsorption capacity showed a better catalytic activity than NPA catalyst.

  6. Hydrogen Production by Steam Reforming of Liquefied Natural Gas (LNG) Over Nickel-Phosphorus-Alumina Xerogel Catalyst Prepared by a Carbon-Templating Epoxide-Driven Sol-Gel Method.

    Science.gov (United States)

    Bang, Yongju; Park, Seungwon; Han, Seung Ju; Yoo, Jaekyeong; Choi, Jung Ho; Kang, Tae Hun; Lee, Jinwon; Song, In Kyu

    2016-05-01

    A nickel-phosphorus-alumina xerogel catalyst was prepared by a carbon-templating epoxide-driven sol-gel method (denoted as CNPA catalyst), and it was applied to the hydrogen production by steam reforming of liquefied natural gas (LNG). For comparison, a nickel-phosphorus-alumina xerogel catalyst was also prepared by a similar method in the absence of carbon template (denoted as NPA catalyst). The effect of carbon template addition on the physicochemical properties and catalytic activities of the catalysts in the steam reforming of LNG was investigated. Both CNPA and NPA catalysts showed excellent textural properties with well-developed mesoporous structure. However, CNPA catalyst retained a more reducible nickel aluminate phase than NPA catalyst. XRD analysis of the reduced CNPA and NPA catalysts revealed that nickel sintering on the CNPA catalyst was suppressed compared to that on the NPA catalyst. From H2-TPD and CH4-TPD measurements of the reduced CNPA and NPA catalysts, it was also revealed that CNPA catalyst with large amount of hydrogen uptake and strong hydrogen-binding sites showed larger amount of methane adsorption than NPA catalyst. In the hydrogen production by steam reforming of LNG, CNPA catalyst with large methane adsorption capacity showed a better catalytic activity than NPA catalyst. PMID:27483798

  7. Ruthenium Bisphosphine Catalyst on Functionalized Silica:Novel Efficient Catalyst for Carbon Dioxide Hydrogenation to Formic Acid

    Institute of Scientific and Technical Information of China (English)

    Yi Ping ZHANG; Jin Hua FEI; Ymg Min YU; Xiao Ming ZHENG

    2006-01-01

    A novel efficient catalyst for the hydrogenation of carbon dioxide to formic acid ruthenium bisphosphine on functionalized silica was in situ synthesized, affording turnover frequency (TOF) of 1190 h-1 at 100% selectivity under 80C with total pressure of 16.0 MPa. The catalyst can be separated from the reaction mixture easily and reused with moderate loss of activity.

  8. INTERACTION-MEDIATED GROWTH OF CARBON NANOTUBES ON ACICULAR SILICA-COATED α-Fe CATALYST BY CHEMICAL VAPOR DEPOSITION

    Institute of Scientific and Technical Information of China (English)

    Qixiang Wang; Guoqing Ning; Fei Wei; Guohua Luo

    2003-01-01

    Multi-walled carbon nanotubes (MWNTs) with 20 nm outer diameter were prepared by chemical vapor deposition of ethylene using ultrafine surface-modified acicular α-Fe catalyst particles. The growth mechanism of MWNTs on the larger catalyst particles are attributed to the interaction between the Fe nanoparticles with the surface-modified silica layer. This interaction-mediated growth mechanism is illustrated by studying the electronic, atomic and crystal properties of surface-modified catalysts and MWNTs products by characterization with X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), thermal gravimetric analysis (TGA) and Raman spectra.

  9. Nitrogen-modified carbon-based catalysts for oxygen reduction reaction in polymer electrolyte membrane fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Subramanian, Nalini P.; Li, Xuguang; Nallathambi, Vijayadurda; Kumaraguru, Swaminatha P.; Colon-Mercado, Hector; Wu, Gang; Lee, Jong-Won; Popov, Branko N. [Center for Electrochemical Engineering, Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208 (United States)

    2009-03-01

    Nitrogen-modified carbon-based catalysts for oxygen reduction were synthesized by modifying carbon black with nitrogen-containing organic precursors. The electrocatalytic properties of catalysts were studied as a function of surface pre-treatments, nitrogen and oxygen concentrations, and heat-treatment temperatures. On the optimum catalyst, the onset potential for oxygen reduction is approximately 0.76 V (NHE) and the amount of hydrogen peroxide produced at 0.5 V (NHE) is approximately 3% under our experimental conditions. The characterization studies indicated that pyridinic and graphitic (quaternary) nitrogens may act as active sites of catalysts for oxygen reduction reaction. In particular, pyridinic nitrogen, which possesses one lone pair of electrons in addition to the one electron donated to the conjugated {pi} bond, facilitates the reductive oxygen adsorption. (author)

  10. Relating FTS Catalyst Properties to Performance

    Science.gov (United States)

    Ma, Wenping; Ramana Rao Pendyala, Venkat; Gao, Pei; Jermwongratanachai, Thani; Jacobs, Gary; Davis, Burton H.

    2016-01-01

    During the reporting period June 23, 2011 to August 31, 2013, CAER researchers carried out research in two areas of fundamental importance to the topic of cobalt-based Fischer-Tropsch Synthesis (FTS): promoters and stability. The first area was research into possible substitute promoters that might be used to replace the expensive promoters (e.g., Pt, Re, and Ru) that are commonly used. To that end, three separate investigations were carried out. Due to the strong support interaction of ?-Al2O3 with cobalt, metal promoters are commonly added to commercial FTS catalysts to facilitate the reduction of cobalt oxides and thereby boost active surface cobalt metal sites. To date, the metal promoters examined have been those up to and including Group 11. Because two Group 11 promoters (i.e., Ag and Au) were identified to exhibit positive impacts on conversion, selectivity, or both, research was undertaken to explore metals in Groups 12 - 14. The three metals selected for this purpose were Cd, In, and Sn. At a higher loading of 25%Co on alumina, 1% addition of Cd, In, or Sn was found to-on average-facilitate reduction by promoting a heterogeneous distribution of cobalt consisting of larger lesser interacting cobalt clusters and smaller strongly interacting cobalt species. The lesser interacting species were identified in TPR profiles, where a sharp low temperature peak occurred for the reduction of larger, weakly interacting, CoO species. In XANES, the Cd, In, and Sn promoters were found to exist as oxides, whereas typical promoters (e.g., Re, Ru, Pt) were previously determined to exist in an metallic state in atomic coordination with cobalt. The larger cobalt clusters significantly decreased the active site density relative to the unpromoted 25%Co/Al2O3 catalyst. Decreasing the cobalt loading to 15%Co eliminated the large non-interacting species. The TPR peak for reduction of strongly interacting CoO in the Cd promoted catalyst occurred at a measurably lower temperature

  11. Multi-Directional Growth of Aligned Carbon Nanotubes Over Catalyst Film Prepared by Atomic Layer Deposition

    Directory of Open Access Journals (Sweden)

    Zhou Kai

    2010-01-01

    Full Text Available Abstract The structure of vertically aligned carbon nanotubes (CNTs severely depends on the properties of pre-prepared catalyst films. Aiming for the preparation of precisely controlled catalyst film, atomic layer deposition (ALD was employed to deposit uniform Fe2O3 film for the growth of CNT arrays on planar substrate surfaces as well as the curved ones. Iron acetylacetonate and ozone were introduced into the reactor alternately as precursors to realize the formation of catalyst films. By varying the deposition cycles, uniform and smooth Fe2O3 catalyst films with different thicknesses were obtained on Si/SiO2 substrate, which supported the growth of highly oriented few-walled CNT arrays. Utilizing the advantage of ALD process in coating non-planar surfaces, uniform catalyst films can also be successfully deposited onto quartz fibers. Aligned few-walled CNTs can be grafted on the quartz fibers, and they self-organized into a leaf-shaped structure due to the curved surface morphology. The growth of aligned CNTs on non-planar surfaces holds promise in constructing hierarchical CNT architectures in future.

  12. Starch saccharification by carbon-based solid acid catalyst

    Science.gov (United States)

    Yamaguchi, Daizo; Hara, Michikazu

    2010-06-01

    The hydrolysis of cornstarch using a highly active solid acid catalyst, a carbon material bearing SO 3H, COOH and OH groups, was investigated at 353-393 K through an analysis of variance (ANOVA) and an artificial neural network (ANN). ANOVA revealed that reaction temperature and time are significant parameters for the catalytic hydrolysis of starch. The ANN model indicated that the reaction efficiency reaches a maximum at an optimal condition (water, 0.8-1.0 mL; starch, 0.3-0.4 g; catalyst, 0.3 g; reaction temperature, 373 K; reaction time, 3 h). The relationship between the reaction and these parameters is discussed on the basis of the reaction mechanism.

  13. Deoxygenation of methanol with carbon monoxide over Fe/ZSM-5 catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Mahay, A.; Lemay, G.; Adnot, A.; Szoeghy, I.M.; Kaliaguine, S.

    1987-02-01

    Deoxygenation is a process of interest in the upgrading of various feedstocks including liquids derived from biomass. Wood liquefaction techniques, especially by pyrolytic processes, yield highly oxygenated products. Two catalytic routes have been proposed for deoxygenation of pyrolytic oils, namely, hydrotreatment with H/sub 2/ or CO + H/sub 2/ over HDS-type catalysts, and dehydration or decarboxylation over zeolite-type acid catalysts. It is proposed in this work to add to the zeolite catalyst a water-gas shift (WGS) function. Over such a bifunctional catalyst it is proposed to feed an oxygenate compound in a stream of carbon monoxide. In such a process, oxygen will be eliminated as CO/sub 2/ rather than H/sub 2/O, and if the WGS active catalyst possesses some hydrogenation properties under the operating conditions, the molecular hydrogen generated by WGS may be reincorporated into the growing hydrocarbon chains. The zeolite component selected is ZSM-5 due to its shape-selectivity properties for the formation of gasoline-range hydrocarbons and its resistance toward coke building. Iron oxide has been chosen as the second component of this dual function catalyst. Another important aspect of this study is the development of a new method for the deposition of iron on ZSM-5. The authors propose to employ ferrocene, which has smaller dimensions than the pore diameter of ZSM-5. Moreover, this type of compound also offers the possibility of controlling the location of iron on the support. A bulky radical, like the dibenzoyl radical, can be added effectively as a substituent on the cyclopentadienyl rings. The large size of this new complex would prevent the diffusion of the organometallic compound into the pores, and consequently, it would allow fixing the iron on only the external surface of the ZSM-5 grains. 37 references.

  14. Graphite-Conjugated Rhenium Catalysts for Carbon Dioxide Reduction

    Energy Technology Data Exchange (ETDEWEB)

    Oh, Seokjoon; Gallagher, James R.; Miller, Jeffrey T.; Surendranath, Yogesh

    2016-02-17

    Condensation of fac-Re(5,6-diamino-1,10-phenanthroline)(CO)(3)Cl to o-quinone edge defects on graphitic carbon surfaces generates graphite-conjugated rhenium (GCC-Re) catalysts that are highly active for CO2 reduction to CO in acetonitrile electrolyte. X-ray photo-electron and X-ray absorption spectroscopies establish the formation of surface-bound Re centers with well-defined coordination environments. GCC-Re species on glassy carbon surfaces display catalytic currents greater than 50 mA cm(-2) with 96 +/- 3% Faradaic efficiency for CO production. Normalized for the number of Re active sites, GCC-Re catalysts exhibit higher turnover frequencies than that of a soluble molecular analogue, fac-Re(1,10-phenanthroline)(CO)(3)Cl, and turnover numbers greater than 12,000. In contrast to the molecular analogue, GCC-Re surfaces display a Tafel slope of 150 mV/decade, indicative of a catalytic mechanism involving rate-limiting one-electron transfer. This work establishes graphite conjugation as a powerful strategy for generating well-defined, tunable, heterogeneous electrocatalysts on ubiquitous graphitic carbon surfaces.

  15. Activated Carbons as Supports for Catalyst%作为催化剂载体的活性炭

    Institute of Scientific and Technical Information of China (English)

    赵波; 韩文锋; 霍超; 刘化章

    2004-01-01

      This paper introduces the advantages of activated carbons as supports for catalysts. The manufacture of the carbons is described briefly, together with their most important chemical and physical properties that are tightly related to catalysts manufacture and use of such catalysts. The treatment methods of activated carbons are also reviewed.%  介绍了活性炭作为催化剂载体的优点、了活性炭的生产方法以及与催化剂的生产和应用密切相关的活性炭的物理及化学性质,并介绍了活性炭的改性处理的方法。

  16. Removal of dye by immobilised photo catalyst loaded activated carbon

    International Nuclear Information System (INIS)

    The ability of activated carbon to adsorb and titanium dioxide to photo degrade organic impurities from water bodies is well accepted. Combination of the two is expected to enhance the removal efficiency due to the synergistic effect. This has enabled activated carbon to adsorb more and at the same time the lifespan of activated carbon is prolonged as the workload of removing organic pollutants is shared between activated carbon and titanium dioxide. Immobilisation is selected to avoid unnecessary filtering of adsorbent and photo catalyst. In this study, mixture of activated carbon and titanium dioxide was immobilised on glass slides. Photodegradation and adsorption studies of Methylene Blue solution were conducted in the absence and presence of UV light. The removal efficiency of immobilised TiO2/ AC was found to be two times better than the removal by immobilised AC or immobilised TiO2 alone. In 4 hours and with the concentration of 10 ppm, TiO2 loaded activated carbon prepared from 1.5 g/ 15.0 mL suspension produced 99.50 % dye removal. (author)

  17. Effect of reduction method on the performance of Pd catalysts supported on activated carbon for the selective oxidation of glucose

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    The effect of the reduction method on the catalytic properties of palladium catalysts supported on activated carbon for the oxidation of D-glucose was examined.The reduction methods investigated include argon glow discharge plasma reduction at room temperature,reduction by flowing hydrogen at elevated temperature,and reduction by formaldehyde at room temperature.The plasma-reduced catalyst shows the smallest metal particles with a narrow size distribution that leads to a much higher activity.The catalyst characteristics show that the plasma reduction increases the amount of oxygen-containing functional groups,which significantly enhances the hydrophilic property of the activated carbon and improves the dispersion of the metal.

  18. Synthesis of carbon nanotubes by CCVD of natural gas using hydrotreating catalysts

    Directory of Open Access Journals (Sweden)

    Ahmed E. Awadallah

    2012-12-01

    Full Text Available Carbon nanotubes have been successfully synthesized using the catalytic chemical vapor deposition (CCVD technique over typical refining hydrotreating catalysts (hydrodesulfurization and hydrodenitrogenation containing Ni–Mo and Co–Mo supported on Al2O3 catalysts at 700°C in a fixed bed horizontal reactor using natural gas as a carbon source. The catalysts and the as-grown CNTs were characterized by transmission electron microscopy, HRTEM, X-ray diffraction patterns, EDX and TGA–DTG. The obtained data clarified that the Ni–Mo catalyst gives higher yield, higher purity and selectivity for CNTs compared to Co–Mo catalyst. XRD, TEM and TGA reveal also that the Ni–Mo catalyst produces mostly CNTs with different diameters whereas the Co–Mo catalyst produces largely amorphous carbon.

  19. Catalytic hydrolysis of ammonia borane for hydrogen generation using cobalt nanocluster catalyst supported on polydopamine functionalized multiwalled carbon nanotube

    International Nuclear Information System (INIS)

    Hydrogen was generated from ammonia borane complex by hydrolysis using cobalt nanocluster catalyst supported on polydopamine functionalized MWCNTs (multi-walled carbon nanotubes). The impregnation-chemical reduction method was used for the preparation of the supported catalyst. The nanocluster catalyst support was formed by in-situ oxidative polymerization of dopamine on the MWCNTs in alkaline solution at room temperature. The structural and physical–chemical properties of the nanocluster catalyst were characterized by FT-IR (Fourier transform infrared spectroscopy), EDX (energy-dispersive X-ray spectroscopy), SEM (scanning electron microscope), XRD (X-ray diffraction) and TEM (transmission electron microscopy). The nanocluster catalyst showed good catalytic activity for the hydrogen generation from aqueous ammonia borane complex. A reusability test to determine the practical usage of the catalyst was also investigated. The result revealed that the catalyst maintained an appreciable catalytic performance and stability in terms of its reusability after three cycle of reuse for the hydrolysis reaction. Also, the activation energy for the hydrolysis of ammonia borane complex was estimated to be 50.41 kJmol−1, which is lower than the values of some of the reported catalyst. The catalyst can be considered as a promising candidate in developing highly efficient portable hydrogen generation systems such as PEMFC (proton exchange membrane fuel cells). - Highlights: • Co/Pdop-o-MWCNT (Pdop functionalized MWCNT supported cobalt nanocluster) catalyst was synthesized for hydrogen generation. • It is an active catalyst for hydrogen generation via hydrolysis of ammonia borane. • It showed good stability in terms of reusability for the hydrogen generation

  20. Hydrogenation of ortho-nitrochlorobenzene on activated carbon supported platinum catalysts

    Institute of Scientific and Technical Information of China (English)

    JIANG Cheng-jun; YIN Hong; CHEN Zhi-rong

    2005-01-01

    Platinum/carbon catalyst is one of the most important catalysts in hydrogenation of ortho-nitrochlorobenzene to 2,2'-dichlorohydrazobenzene. The preparation process and the supports of catalysts are studied in this paper. Raw materials and preparation procedure of the activated carbon have great influences on the compositions and surface structure of platinum/carbon catalysts. Platinum catalysts supported on activated carbon with high purity, high surface area, large pore volume and appropriate pore structure usually exhibit higher activities for hydrogenation of ortho-nitrochlorobenzene to 2,2'-dichlorohydrazobenzene.The catalyst prepared from H2PtCl6 with pH=3 shows greater catalytic performance than those prepared under other conditions.

  1. Nano carbon supported platinum catalyst interaction behavior with perfluorosulfonic acid ionomer and their interface structures

    DEFF Research Database (Denmark)

    Andersen, Shuang Ma

    2016-01-01

    behavior of Nafion ionomer on platinized carbon nano fibers (CNFs), carbon nano tubes (CNTs) and amorphous carbon (Vulcan). The interaction is affected by the catalyst surface oxygen groups as well as porosity. Comparisons between the carbon supports and platinized equivalents are carried out. It reveals......, the ionomer may have an adsorption preference to the platinum nano particle rather than to the overall catalyst. This was verified by a close examination on the decomposition temperature of the carbon support and the ionomer. The electrochemical stability of the catalyst ionomer composite electrode suggests...

  2. Study of Supported Nickel Catalysts Prepared by Aqueous Hydrazine Method. Hydrogenating Properties and Hydrogen Storage: Support Effect. Silver Additive Effect

    International Nuclear Information System (INIS)

    We have studied Ni or NiAg nano-particles obtained by the reduction of nickel salts (acetate or nitrate) by hydrazine and deposited by simple or EDTA-double impregnation on various supports (γ-Al2O3, amorphous or crystallized SiO2, Nb2O5, CeO2 and carbon). Prepared catalysts were characterized by different methods (XRD, XPS, low temperature adsorption and desorption of N2, FTIR and FTIR-Pyridine, TEM, STEM, EDS, H2-TPR, H2-adsorption, H2-TPD, isopropanol decomposition) and tested in the gas phase hydrogenation of benzene or as carbon materials in the hydrogen storage at room temperature and high pressure. The catalysts prepared exhibited better dispersion and activity than classical catalysts. TOF's of NiAg/SiO2 or Ni/carbon catalysts were similar to Pt catalysts in benzene hydrogenation. Differences in support acidity or preparation method and presence of Ag as metal additive play a crucial role in the chemical reduction of Ni by hydrazine and in the final properties of the materials. Ni/carbon catalysts could store significant amounts of hydrogen at room temperature and high pressure (0.53%/30 bars), probably through the hydrogen spillover effect. (author)

  3. Natural Mineral-marine Manganese Nodule as a Novel Catalyst for the Synthesis of Carbon Nanotubes

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    Multi-walled carbon nanotubes were fabricated by the pyrolysis of acetylene with naturally occurring marine manganese nodules as a novel catalyst at an elevated temperature.The nanotube product was examined by transmission electron microscopy.The method is expected to be the simplest one to synthesize carbon nanotubes due to unnecessary synthesis of catalyst.

  4. Co-production of hydrogen and carbon nanofibers from methane decomposition over zeolite Y supported Ni catalysts

    International Nuclear Information System (INIS)

    Highlights: • Methane cracking requires an optimum temperature range of 550–600 °C for H2 yield. • At 550 and 600 °C, catalyst showed longer activity for the whole test. • At 600 °C, a 614.25 gc/gNi of carbon was obtained using 30% Ni/Y zeolite catalysts. • Produced filamentous carbon has the same diameter as the metallic nickel itself. • VHSV has reverse and non-linear relevancy to the weight of Ni/Y zeolite catalyst. - Abstract: The objective of this paper is to study the influences of different operating conditions on the hydrogen formation and properties of accumulated carbon from methane decomposition using zeolite Y supported 15% and 30% Ni, respectively, at a temperature range between 500 and 650 °C in a pilot scale fixed bed reactor. The temperature ramp was showed a significant impact on the thermo-catalytic decomposition (TCD) of methane. An optimum temperature range of 550–600 °C were required to attain the maximum amount of methane conversion and revealed that at 550 and 600 °C, catalyst showed longer activity for the whole studied of experimental runs. Additionally, at 550 °C, the methane decomposition is two times longer for 30% Ni/Y zeolite than that for 15% Ni/Y zeolite catalyst, whereas it is almost three times higher at 500 °C. A maximum carbon yield of 614.25 and 157.54 gc/gNi were reported after end of the complete reaction at 600 °C with 30% and 15% Ni/Y zeolite catalyst, respectively. From BET, TPD, and XRD analysis, we had reported that how the chemistry between the TCD of methane and metal content of the catalysts could significantly affect the hydrogen production as well as carbon nano-fibers. TEM analysis ensured that the produced carbon had fishbone type structures with a hollow core and grew from crystallites of Ni anchored on the external surface of the catalysts and irrespective of the metal loadings, the whisker types of nano filaments were formed as confirmed from FESEM analysis. Nevertheless, the effect of

  5. Thermal carbonization of nanoporous silicon: Formation of carbon nanofibres without a metal catalyst

    Indian Academy of Sciences (India)

    Gunjan Aggarwal; Prabhash Mishra; Bipin Joshi; S S Islam

    2014-09-01

    An interesting phenomenon is observed while carrying out thermal carbonization of porous silicon (PS) with an aim to arrest the natural surface degradation, and it is a burning issue for PS-based device applications. A tubular carbon structure has been observed on the PS surface. Raman, Fourier transform infrared spectroscopy (FTIR) and electron microscope studies, revealed that the tubular structure is nothing but amorphous carbon nanofibres sprouted within the pores in the absence of a metal catalyst, for which a suitable explanation is proposed.

  6. Electron paramagnetic resonance investigation of purified catalyst-free single-walled carbon nanotubes.

    Science.gov (United States)

    Zaka, Mujtaba; Ito, Yasuhiro; Wang, Huiliang; Yan, Wenjing; Robertson, Alex; Wu, Yimin A; Rümmeli, Mark H; Staunton, David; Hashimoto, Takeshi; Morton, John J L; Ardavan, Arzhang; Briggs, G Andrew D; Warner, Jamie H

    2010-12-28

    Electron paramagnetic resonance of single-walled carbon nanotubes (SWCNTs) has been bedevilled by the presence of paramagnetic impurities. To address this, SWCNTs produced by laser ablation with a nonmagnetic PtRhRe catalyst were purified through a multiple step centrifugation process in order to remove amorphous carbon and catalyst impurities. Centrifugation of a SWCNT solution resulted in sedimentation of carbon nanotube bundles containing clusters of catalyst particles, while isolated nanotubes with reduced catalyst particle content remained in the supernatant. Further ultracentrifugation resulted in highly purified SWCNT samples with a narrow diameter distribution and almost no detectable catalyst particles. Electron paramagnetic resonance (EPR) signals were detected only for samples which contained catalyst particles, with the ultracentrifuged SWCNTs showing no EPR signal at X-band (9.4 GHz) and fields < 0.4 T. PMID:21082779

  7. Catalytic activity vs. size correlation in platinum catalysts of PEM fuel cells prepared on carbon black by different methods

    Energy Technology Data Exchange (ETDEWEB)

    Nores-Pondal, F.J.; Granada, M.; Corti, H.R. [Departamento de Fisica de la Materia Condensada, Centro Atomico Constituyentes, Comision Nacional de Energia Atomica (CNEA), General Paz 1499, 1650 San Martin, Buenos Aires (Argentina); Vilella, I.M.J.; de Miguel, S.R.; Scelza, O.A. [Instituto de Investigaciones en Catalisis y Petroquimica (INCAPE), Facultad de Ingenieria Quimica (Universidad Nacional del Litoral) - CONICET, Santiago del Estero 2654, 3000 Santa Fe (Argentina); Troiani, H. [Departamento de Fisica, Centro Atomico Bariloche, Comision Nacional de Energia Atomica (CNEA), Av. Bustillo 9500, 8400 San Carlos de Bariloche (Argentina)

    2009-10-15

    In this work nanoparticulated platinum catalysts have been prepared on carbon Vulcan XC-72 using three methods starting with chloroplatinic acid as a precursor: (i) formic acid as a reductor agent; (ii) impregnation method followed by reduction in hydrogen atmosphere at moderated temperature; and (iii) microwave-assisted reduction in ethylene glycol. The catalytic and size studies were also performed on a commercial Pt catalyst (E-Tek, De Nora). The characterization of the particle size and distribution was performed by means of transmission electron microscopy (TEM) and X-ray diffraction (XRD). The characterizations of the catalytic and electrocatalytic properties of the catalysts were determined by studying the cyclohexane dehydrogenation reaction (CHD) and the behavior under cyclic voltammetry (CV) in sulfuric acid solutions. The measured electrochemical activity, along with the hydrogen chemisorption of the catalysts allows the estimation of effective particle sizes, which are much larger than those measured by TEM and XRD. The catalysts prepared by reduction with formic acid and ethylene glycol (microwave-assisted) show electrochemical activities very close to those of the commercial catalyst, and are almost insensitive to the Pt dispersion or Pt particle size. The chemical activity in CHD correlates well with the metallic dispersion determined by hydrogen chemisorption, indicating similar accesibility of H{sub 2} and cyclohexane to the catalyst surface. (author)

  8. Synthesis and Characterization of Carbon nanofibers on Co and Cu Catalysts by Chemical Vapor Deposition

    Energy Technology Data Exchange (ETDEWEB)

    Park, Eunsil; Kim, Jongwon; Lee, Changseop [Keimyung Univ., Daegu (Korea, Republic of)

    2014-06-15

    This study reports on the synthesis of carbon nanofibers via chemical vapor deposition using Co and Cu as catalysts. In order to investigate the suitability of their catalytic activity for the growth of nanofibers, we prepared catalysts for the synthesis of carbon nanofibers with Cobalt nitrate and Copper nitrate, and found the optimum concentration of each respective catalyst. Then we made them react with Aluminum nitrate and Ammonium Molybdate to form precipitates. The precipitates were dried at a temperature of 110 .deg. C in order to be prepared into catalyst powder. The catalyst was sparsely and thinly spread on a quartz tube boat to grow carbon nanofibers via thermal chemical vapor deposition. The characteristics of the synthesized carbon nanofibers were analyzed through SEM, EDS, XRD, Raman, XPS, and TG/DTA, and the specific surface area was measured via BET. Consequently, the characteristics of the synthesized carbon nanofibers were greatly influenced by the concentration ratio of metal catalysts. In particular, uniform carbon nanofibers of 27 nm in diameter grew when the concentration ratio of Co and Cu was 6:4 at 700 .deg. C of calcination temperature; carbon nanofibers synthesized under such conditions showed the best crystallizability, compared to carbon nanofibers synthesized with metal catalysts under different concentration ratios, and revealed 1.26 high amorphicity as well as 292 m{sup 2}g{sup -1} high specific surface area.

  9. New Rh-ZnO/Carbon Nanotubes Catalyst for Methanol Synthesis

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    A new catalyst for methanol synthesis, ZnO-promoted rhodium supported on carbon nanotubes, was developed. It was found that the Rh-ZnO/CNTs catalyst had high activity of 411.4 mg CH3OH/g/cat/h and selectivity of 96.7 % for methanol at 1 MPa and 523 K. The activity of this catalyst is much higher than that of NC 207 catalyst at the same reaction conditions. It was suggested that the multi-walled structure CNTs favored both the couple transfer of the proton and electron over the surface of the catalyst and the uptake of hydrogen which was favorable to methanol synthesis.

  10. Synergistic effect of carbon nanofiber/nanotube composite catalyst on carbon felt electrode for high-performance all-vanadium redox flow battery.

    Science.gov (United States)

    Park, Minjoon; Jung, Yang-jae; Kim, Jungyun; Lee, Ho il; Cho, Jeaphil

    2013-10-01

    Carbon nanofiber/nanotube (CNF/CNT) composite catalysts grown on carbon felt (CF), prepared from a simple way involving the thermal decomposition of acetylene gas over Ni catalysts, are studied as electrode materials in a vanadium redox flow battery. The electrode with the composite catalyst prepared at 700 °C (denoted as CNF/CNT-700) demonstrates the best electrocatalytic properties toward the V(2+)/V(3+) and VO(2+)/VO2(+) redox couples among the samples prepared at 500, 600, 700, and 800 °C. Moreover, this composite electrode in the full cell exhibits substantially improved discharge capacity and energy efficiency by ~64% and by ~25% at 40 mA·cm(-2) and 100 mA·cm(-2), respectively, compared to untreated CF electrode. This outstanding performance is due to the enhanced surface defect sites of exposed edge plane in CNF and a fast electron transfer rate of in-plane side wall of the CNT.

  11. Effect of samarium on methanation resistance of activated carbon supported ruthenium catalyst for ammonia synthesis

    Institute of Scientific and Technical Information of China (English)

    周春晖; 祝一锋; 刘化章

    2010-01-01

    The effects of samarium(Sm) on carbon-methanation and catalytic activity of the Ba-Ru-K/AC (active carbon) catalyst for ammonia synthesis were investigated. The addition of samarium improved significantly the activity and stability of the catalyst. The results of temperature-programmed desorption (H2-TPD) and in-situ-TPSR FTIR indicated that samarium impeded the adsorption of hydrogen on the catalyst surface, thus leading to the high catalytic activity and resistance to carbon-methanation. XRD patterns reve...

  12. Measurement of a new parameter representing the gas transport properties of the catalyst layers of polymer electrolyte fuel cells.

    Science.gov (United States)

    Iden, Hiroshi; Ohma, Atsushi; Tokunaga, Tomomi; Yokoyama, Kouji; Shinohara, Kazuhiko

    2016-05-14

    The optimization of the catalyst layers is necessary for obtaining a better fuel cell performance and reducing fuel cell cost. Although the ionomer coverage of the Pt catalyst is said to be a key parameter in this regard, the proportion of Pt either directly or indirectly covered by the ionomer is thought to be an important parameter with regard to gas transport (indirectly covered Pt: its gas transport paths are completely blocked by the ionomer even if it does not directly cover Pt). In this study, a new technique has been developed for evaluating the proportion of Pt covered indirectly or directly by the ionomer, which is defined as the "capped proportion", based on the carbon monoxide (CO) adsorption properties at different temperatures. The validity of the method was thoroughly examined by identifying the CO adsorption properties of the components of the catalyst layers. The capped proportion and oxygen transport resistance in the catalyst layers showed a good correlation, indicating that the capped proportion is a dominant factor of oxygen transport resistance. This technique thus enables the evaluation of the dominant factor of the gas transport properties of the catalyst layers. The method has another significant advantage in that it does not require a membrane electrode assembly, let alone electrochemical measurement, which should be helpful for catalyst layer optimization.

  13. Synthesis and growth kinetics of carbon nanocoils using Sn-Fe-O xerogel film catalyst

    International Nuclear Information System (INIS)

    Carbon nanocoils (CNCs) were synthesized by a chemical vapor deposition method using tin-iron-oxide (Sn-Fe-O) xerogel film catalyst. The Sn-Fe-O catalyst was prepared by a low-cost sol–gel method using stannous acetate and ferric acetate as precursors. The growth kinetics of CNCs were monitored by a thermogravimetric analyzer, and the experimental result was correlated using one-dimensional tip growth kinetic model. The kinetic model consists of three steps: (1) dissociative chemisorption of acetylene and formation of encapsulating carbon on a leading face of the catalyst, (2) diffusion and reduction of Sn-Fe-O catalyst in bulk structure, and (3) carbon cluster nucleation on a tailing face of the catalyst. (paper)

  14. Ni supported on activated carbon as catalyst for flue gas desulfurization

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    A series of Ni supported on activated carbon are prepared by excessive impregnation and the desulfurization activity is investigated. It has been shown that the activated carbon-supported Ni is an efficient solid catalyst for flue gas desulfurization. The activated carbon treated by HNO3 exhibits high desulfurization activity, and different amounts of loaded-Ni on activated carbon significantly influence the desulfurization activity. The catalysts are studied by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The results of XRD and XPS indicate that the activated carbon treated by HNO3 can increase oxygen-containing functional groups. Ni on activated carbon after calcination at 800 °C shows major Ni phase and minor NiO phase, and with increasing Ni content on activated carbon, Ni phase increases and affects the desulfurization activity of the catalyst, which proves that Ni is the main active phase.

  15. Preparation of Carbon Nanotubes from Methane on Ni/Cu/A1 Catalyst

    Institute of Scientific and Technical Information of China (English)

    Renzhong Wei; Fengyi Li; Yan Ju

    2005-01-01

    A series of Ni/Cu/Al catalyst samples were prepared by the co-precipitation method. Carbon nanotubes with large inner diameters are successfully synthesized from methane on Ni/Cu/Al catalyst by adding sodium carbonate. The effects of the copper content and amounts of sodium carbonate on the morphology and microstructures of carbon nanotubes were investigated by CO adsorption and TEM technique. The experimental results showed that copper can influence both the catalytic activity and catalyst life. Best result was obtained when the copper content was 15%. Addition of sodium carbonate favors the formation of carbon nanotubes with large inner diameters. The growth mechanism of carbon nanotubes with large inner diameter is discussed.

  16. A New Process for Synthesis of Dimethyl Carbonate from Ethylene Carbonate and Methanol without any Catalyst under Supercritical Conditions

    Institute of Scientific and Technical Information of China (English)

    Xiu Juan FENG; Xiao Gang LI; Ren HE; Hui ZHOU

    2005-01-01

    Dimethyl carbonate was synthesized by transesterification reaction between ethylene carbonate and methanol under supercritical conditions without any catalyst. Experimental results showed that the residence time and the molar ratio of methanol to ethylene carbonate all can affect the conversion of ethylene carbonate. When the molar ratio of methanol to ethylene carbonate was 8:1, 81.2 % conversion can be achieved at 9.0 MPa and 250℃ after 8 h.

  17. In situ adsorption-catalysis system for the removal of o-xylene over an activated carbon supported Pd catalyst

    Institute of Scientific and Technical Information of China (English)

    HUANG Shaoyong; ZHANG Changbin; HE Hong

    2009-01-01

    An activated carbon (AC) supported Pd catalyst was used to develop a highly efficient in situ adsorption-catalysis system for the removal of low concentrations of o-xylene. In this study, three kinds of Pd/AC catalysts were prepared and tested to investigate the synergistic efficiency between adsorption and catalysis for o-xylene removal. The Pd/AC catalyst was first used as an adsorbent to concentrate dilute o-xylene at low temperature. After saturated adsorption, the adsorbed o-xylene was oxidized to CO2 and H2O by raising the temperature of the catalyst bed. The results showed that more than 99% of the adsorbed o-xylene was completely oxidized to CO2 over a 5% Pd/AC catalyst at 140℃. Brunauer-Emmett-Teller (BET) analysis, scanning electron microscopy (SEM), temperature-programmed desorption (TPD), and temperature-programmed oxidation (TPO) were applied to investigate the physical properties of o-xylene adsorption-desorption and the in situ adsorption-catalysis activity of the AC support and Pd/AC catalyst. A synergistic relationship between the AC support and the active Pd species for the removal of low concentrations of o-xylene was established.

  18. Carbon as a hard template for nano material catalysts

    Institute of Scientific and Technical Information of China (English)

    Kake Zhu; Junming Sun; He Zhang; Jun Liu; Yong Wang

    2012-01-01

    As one of the naturally abundant elements,carbon can present in different molecular structures (allotropes) and thus lead to various physical/chemical properties of carbon-based materials which have found wide applications in a variety of fields including electrochemistry,optical,adsorption and catalysis,etc.On the other hand,its different allotropes also endow carbon-based materials with various morphostructures,which have been recently explored to prepare oxides and zeolites/zeotypes with tailored structures.In this review,we mainly summarize the recent advances in using carbon materials as hard templates to synthesize structural materials.Specifically,we focus on the development in the synthetic strategies,such as endotemplating,exotemplating approaches and using carbon materials as chemical reagents for the synthesis of metal carbides or nitrides,with an emphasis laid on the control of morphostructure.Meanwhile,the applications of the obtained materials will be highlighted,especially,in the field of heterogeneous catalysis where enhanced performances have been achieved with the materials derived from carbon-templated methods.

  19. Exposure of metallic copper surface on Cu-Al2O3-carbon catalysts

    NARCIS (Netherlands)

    Menon, P.G.; Prasad, J.

    1970-01-01

    The bifunctional nature of Cu---Al2O3-on-carbon catalysts, used in the direct catalytic conversion of ethanol to ethyl acetate, prompted an examination of the dispersion of Cu on the composite catalyst. For this, the N2O-method of Osinga et al. for estimation of bare metallic copper surface on compo

  20. Mechanisms of oxygen reduction reactions for carbon alloy catalysts via first principles molecular dynamics

    International Nuclear Information System (INIS)

    Carbon alloy catalysts (CACs) are one of promising candidates for platinum-substitute cathode catalysts for polymer electrolyte fuel cells. We have investigated possible mechanisms of oxygen reduction reactions (ORRs) for CACs via first-principles-based molecular dynamics simulations. In this contribution, we review possible ORRs at likely catalytic sites of CACs suggested from our simulations. (author)

  1. Catalyst functionalized buffer sorbent pebbles for rapid separation of carbon dioxide from gas mixtures

    Energy Technology Data Exchange (ETDEWEB)

    Aines, Roger D

    2015-03-31

    A method for separating CO.sub.2 from gas mixtures uses a slurried media impregnated with buffer compounds and coating the solid media with a catalyst or enzyme that promotes the transformation of CO.sub.2 to carbonic acid. Buffer sorbent pebbles with a catalyst or enzyme coating are provided for rapid separation of CO.sub.2 from gas mixtures.

  2. Catalyst Activation by Microplasma for Carbon Nanofiber Synthesis in a Microreactor

    NARCIS (Netherlands)

    Agiral, Anil; Lefferts, Leon; Gardeniers, J.G.E.

    2009-01-01

    A dielectric barrier discharge is generated by flowing helium and hydrogen through a microreactor capillary which contains a coating of Ni/alumina catalyst to activate carbon nanofiber (CNF) synthesis. Optical and electrical measurements have been done to characterize the discharge during catalyst t

  3. Carbon Nanofiber Supported Transition-Metal Carbide Catalysts for the Hydrodeoxygenation of Guaiacol

    NARCIS (Netherlands)

    Jongerius, A.; Gosselink, R.W.; Dijkstra, J.; Bitter, J.H.; Bruijnincx, P.C.A.; Weckhuysen, B.M.

    2013-01-01

    Hydrodeoxygenation (HDO) studies over carbon nanofiber-supported (CNF) W2C and Mo2C catalysts were performed on guaiacol, a prototypical substrate to evaluate the potential of a catalyst for valorization of depolymerized lignin streams. Typical reactions were executed at 55 bar hydrogen pressure ove

  4. Novel Carbon Nanotubes-supported NiB Amorphors Alloy Catalyst for Benzene Hydrogenation

    Institute of Scientific and Technical Information of China (English)

    Mei Hua YANG; Rong Bin ZHANG; Feng Yi LI

    2004-01-01

    The NiB amorphous alloy catalysts supported on CNTs and alumina were prepared by impregnation and chemical reduction. The gas-phase benzene hydrogenation was used as a probe reaction to evaluate the catalytic activity. The result showed that the NiB amorphous alloy catalyst supported on carbon nanotubes exhibited higher activity than that supported on alumina.

  5. Catalyst functionalized buffer sorbent pebbles for rapid separation of carbon dioxide from gas mixtures

    Science.gov (United States)

    Aines, Roger D.

    2013-03-12

    A method for separating CO.sub.2 from gas mixtures uses a slurried media impregnated with buffer compounds and coating the solid media with a catalyst or enzyme that promotes the transformation of CO.sub.2 to carbonic acid. Buffer sorbent pebbles with a catalyst or enzyme coating are provided for rapid separation of CO.sub.2 from gas mixtures.

  6. Carbon Xerogel-supported Iron as a Catalyst in Combustion Synthesis of Carbon Fibrous Nanostructures

    Institute of Scientific and Technical Information of China (English)

    Wojciech Kiciriski; Joanna Lasota

    2012-01-01

    The catalytically assisted self-propagating high-temperature synthesis of carbon fibrous nanostructures, where the iron-doped colloidal carbon xerogel is proposed as a catalyst system, was examined. The carbon xerogel was prepared through carbonization of an iron doped organic xerogel at temperatures ranging from 600 to 1050℃. The reaction between calcium carbide and hexachloroethane in the presence of sodium azide is exothermic enough to proceed at a high temperature, self-sustaining regime. The combustion reactions of those mixtures enriched with iron-doped carbon xerogels were conducted in a stainless steel reactor---calorimetric bomb under an initial pressure of 1 MPa of argon. Scanning electron microscopy analysis of the combustion products revealed low yield of various type of carbon fibers (presumably nanotubes), which grew via the tip-growth mechanism. The fibrous nanostructures were found in the vicinity of the spot of ignition, while in the outer and cooler area of the reactor, dusty products with soot-like morphology dominated. No significant correlation between the pyrolysis temperature of the carbon xerogel and the morphology of the obtained carbon fibrous nanostructures was observed.

  7. The effect of alkaline doped catalysts on the CVD synthesis of carbon nanotubes

    DEFF Research Database (Denmark)

    Nemeth, Krisztian; Nemeth, Zoltan; Fejes, Dora;

    2011-01-01

    The aim of this work was to develop new doped catalysts for chemical vapour deposition (CVD) synthesis in order to increase the quantity and quality of carbon nanotubes (CNTs). Doping compounds such as CsBr, CsCl, KBr and KCl were used to reach higher carbon deposit and carbon yield. The amount o...

  8. Microwave-assisted synthesis of high-loading, highly dispersed Pt/carbon aerogel catalyst for direct methanol fuel cell

    Indian Academy of Sciences (India)

    Zhijun Guo; Hong Zhu; Xinwei Zhang; Fanghui Wang; Yubao Guo; Yongsheng Wei

    2011-06-01

    A Pt supported on carbon aerogel catalyst has been synthesized by the microwave-assisted polyol process. The Pt supported on carbon aerogel catalyst was characterized by high resolution transmission electron microscopy and X-ray diffraction. The results show a uniform dispersion of spherical Pt nanoparticles 2.5–3.0 nm in diameter. Cyclic voltammetry and chronoamperometry were used to evaluate the electrocatalytic activity of the Pt/carbon aerogel catalyst for methanol oxidation at room temperature. The Pt/carbon aerogel catalyst shows higher electrochemical catalytic activity and stability for methanol oxidation than a commercial Pt/C catalyst of the same Pt loading.

  9. Composite catalysts supported on modified carbon substrates and methods of making the same

    Science.gov (United States)

    Popov, Branko N.; Subramanian, Nalini; Colon-Mercado, Hector R.

    2009-11-17

    A method of producing a composite carbon catalyst is generally disclosed. The method includes oxidizing a carbon precursor (e.g., carbon black). Optionally, nitrogen functional groups can be added to the oxidized carbon precursor. Then, the oxidized carbon precursor is refluxed with a non-platinum transitional metal precursor in a solution. Finally, the solution is pyrolyzed at a temperature of at least about 500.degree. C.

  10. Efficient catalyst-free chemical fixation of carbon dioxide into 2-oxazolidinones under supercritical condition

    Institute of Scientific and Technical Information of China (English)

    Jing Xiu Xu; Jin Wu Zhao; Zhen Bin Jia

    2011-01-01

    4-Methylene-1,3-oxazolidin-2-ones can be synthesized from propargylic alcohols, primary amines and carbon dioxide under supercritical condition in the absence of any additional catalyst and solvent. Various propargylic alcohols and primary amines were examined.

  11. Highly active catalyst for vinyl acetate synthesis by modified activated carbon

    Institute of Scientific and Technical Information of China (English)

    Chun Yan Hou; Liang Rong Feng; Fa Li Qiu

    2009-01-01

    A new zinc acetate catalyst which was prepared from modified activated carbon exhibited extreme activity towards the synthesis of vinyl acetate. The activated carbon was modified by nitric acid, vitriol and peroxyacetic acid (PAA). The effect on specific area, structure, pH and surface acidity groups of carriers by modification was discussed. Amount of carbonyl and carboxyl groups in activated carbon was increased by peroxyacetic acid treatment. The productivity of the new catalyst was 14.58% higher than that of catalyst prepared using untreated activated carbon. The relationship between amount of carbonyl and carboxyl groups (m) and catalyst productivity (P) was P = 1.83 + 2.26 x 10-3e3.17m. Reaction mechanism was proposed.

  12. Renewable phenols production by catalytic microwave pyrolysis of Douglas fir sawdust pellets with activated carbon catalysts.

    Science.gov (United States)

    Bu, Quan; Lei, Hanwu; Wang, Lu; Wei, Yi; Zhu, Lei; Liu, Yupeng; Liang, Jing; Tang, Juming

    2013-08-01

    The effects of different activated carbon (AC) catalysts based on various carbon sources on products yield and chemical compositions of upgraded pyrolysis oils were investigated using microwave pyrolysis of Douglas fir sawdust pellets. Results showed that high amounts of phenols were obtained (74.61% and 74.77% in the upgraded bio-oils by DARCO MRX (wood based) and DARCO 830 (lignite coal based) activated carbons, respectively). The catalysts recycling test of the selected catalysts indicated that the carbon catalysts can be reused for at least 3-4 times and produced high concentrations of phenol and phenolic compounds. The chemical reaction mechanism for phenolics production during microwave pyrolysis of biomass was analyzed.

  13. Electro-oxidation of Ethanol on Carbon Supported PtSn and PtSnNi Catalysts

    Directory of Open Access Journals (Sweden)

    Nur Hidayati

    2016-03-01

    Full Text Available Even though platinum is known as an active electro-catalyst for ethanol oxidation at low temperatures (< 100 oC, choosing the electrode material for ethanol electro-oxidation is a crucial issue. It is due to its property which easily poisoned by a strong adsorbed species such as CO. PtSn-based electro-catalysts have been identified as better catalysts for ethanol electro-oxidation. The third material is supposed to improved binary catalysts performance. This work presents a study of the ethanol electro-oxidation on carbon supported Pt-Sn and Pt-Sn-Ni catalysts. These catalysts were prepared by alcohol reduction. Nano-particles with diameters between 2.5-5.0 nm were obtained. The peak of (220 crystalline face centred cubic (fcc Pt phase for PtSn and PtSnNi alloys was repositioned due to the presence of Sn and/or Ni in the alloy. Furthermore, the modification of Pt with Sn and SnNi improved ethanol and CO electro-oxidation. Copyright © 2016 BCREC GROUP. All rights reserved Received: 10th November 2015; Revised: 1st February 2016; Accepted: 1st February 2016 How to Cite: Hidayati, N., Scott, K. (2016. Electro-oxidation of Ethanol on Carbon Supported PtSn and PtSnNi Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 11 (1: 10-20. (doi:10.9767/bcrec.11.1.394.10-20 Permalink/DOI: http://dx.doi.org/10.9767/bcrec.11.1.394.10-20

  14. Controlling the number of walls in multi walled carbon nanotubes/alumina hybrid compound via ball milling of precipitate catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Nosbi, Norlin [School of Materials and Mineral Resources Engineering, Engineering Campus, Universiti Sains Malaysia (USM), 14300 Nibong Tebal, Seberang Perai Selatan, Pulau Pinang (Malaysia); Akil, Hazizan Md, E-mail: hazizan@usm.my [School of Materials and Mineral Resources Engineering, Engineering Campus, Universiti Sains Malaysia (USM), 14300 Nibong Tebal, Seberang Perai Selatan, Pulau Pinang (Malaysia); Cluster for Polymer Composite (CPC), Science and Engineering Research Centre, Engineering Campus, Universiti Sains Malaysia (USM), 14300 Nibong Tebal, Seberang Perai Selatan, Pulau Pinang (Malaysia)

    2015-06-15

    Graphical abstract: - Highlights: • We report that, to manipulate carbon nanotubes geometry and number of walls are by controlling the precipitate catalyst size. • Number of walls and geometry effects depend on the milling time of the precipitate catalyst. • Increasing milling of time will decrease the carbon nanotubes number of walls. • Increasing milling of time will increase the carbon nanotubes thermal conductivity. - Abstract: This paper reports the influence of milling time on the structure and properties of the precipitate catalyst of multi walled carbon nanotubes (MWCNT)/alumina hybrid compound, produced through the chemical vapour deposition (CVD) process. For this purpose, light green precipitate consisted of aluminium, nickel(II) nitrate hexahydrate and sodium hydroxide mixture was placed in a planetary mill equipped with alumina vials using alumina balls at 300 rpm rotation speed for various milling time (5–15 h) prior to calcinations and CVD process. The compound was characterized using various techniques. Based on high-resolution transmission electron microscopy analysis, increasing the milling time up to 15 h decreased the diameter of MWCNT from 32.3 to 13.1 nm. It was noticed that the milling time had a significant effect on MWCNT wall thickness, whereby increasing the milling time from 0 to 15 h reduced the number of walls from 29 to 12. It was also interesting to note that the carbon content increased from 23.29 wt.% to 36.37 wt.% with increasing milling time.

  15. Carbon supported Cu-Pd nanoparticles as anode catalyst for direct borohydride-hydrogen peroxide fuel cells

    International Nuclear Information System (INIS)

    Carbon supported Cu-Pd bimetallic nanoparticles were prepared by a successive reduction method in aqueous solution and used as anode electrocatalyst for direct borohydride-hydrogen peroxide fuel cell (DBHFC). The physical and electrochemical properties of the as-prepared electrocatalysts are investigated by transmission electron microscopy (TEM), X-ray diffraction (XRD), cyclic voltammetry (CV), chronopotentiometry (CP), linear sweep voltammetry (LSV) and fuel cell test. The results show that the size of the crystallite is around 12.5 nm, the Cu1Pd1/C catalyst presents the highest catalytic activity among all the resultant catalysts, and the DBHFC using Cu1Pd1/C as anode catalyst and Pt mesh (1 cm × 1 cm) as cathode electrode obtains the maximum power density as high as 39.8 mW cm-2 at a discharge current density of 80.1 mA cm-2 at 20 °C

  16. Carbon nanotubes-Nafion composites as Pt-Ru catalyst support for methanol electro-oxidation in acid media

    Institute of Scientific and Technical Information of China (English)

    Shengzhou Chen; Fei Ye; Weiming Lin

    2009-01-01

    Carbon nanotubes-Nafion (CNTs-Nafion) composites were prepared by impregnated CNTs with Nafion in ethanol solution and characterized by FT-IR. Pt-Ru catalysts supported on CNTs-Nafion composites were synthesized by microwave-assisted polyol process. The physical and electrochemical properties of the catalysts were characterized by X-ray diffraction (XRD), transmission electron microscope (TEM), CO stripping voltammetry, cyclic voltammetry (CV) and chronoamperometry (CA). The results showed that the Nafion incorporation in CNTs-Nafion composites did not significantly alter the oxygen-containing groups on the CNTs surface. The Pt-Ru catalyst supported on CNTs-Nafion composites with 2 wt% Nafion showed good dispersion and the best CO oxidation and methanol electro-oxidation activities.

  17. Interfacial Cu+ promoted surface reactivity: Carbon monoxide oxidation reaction over polycrystalline copper-titania catalysts

    Science.gov (United States)

    Senanayake, Sanjaya D.; Pappoe, Naa Adokaley; Nguyen-Phan, Thuy-Duong; Luo, Si; Li, Yuanyuan; Xu, Wenqian; Liu, Zongyuan; Mudiyanselage, Kumudu; Johnston-Peck, Aaron C.; Frenkel, Anatoly I.; Heckler, Ilana; Stacchiola, Dario; Rodriguez, José A.

    2016-10-01

    We have studied the catalytic carbon monoxide (CO) oxidation (CO + 0.5O2 → CO2) reaction using a powder catalyst composed of both copper (5 wt.% loading) and titania (CuOx-TiO2). Our study was focused on revealing the role of Cu, and the interaction between Cu and TiO2, by systematic comparison between two nanocatalysts, CuOx-TiO2 and pure CuOx. We interrogated these catalysts under in situ conditions using X-ray diffraction (XRD), X-ray absorption fine structure (XAFS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to probe the structure and electronic properties of the catalyst at all stages of the reaction and simultaneously probe the surface states or intermediates of this reaction. With the aid of several ex situ characterization techniques including transmission electron microscopy (TEM), the local catalyst morphology and structure were also studied. Our results show that a CuOx-TiO2 system is more active than bulk CuOx for the CO oxidation reaction due to its lower onset temperature and better stability at higher temperatures. Our results also suggest that surface Cu+ species observed in the CuOx-TiO2 interface are likely to be a key player in the CO oxidation mechanism, while implicating that the stabilization of this species is probably associated with the oxide-oxide interface. Both in situ DRIFTS and XAFS measurements reveal that there is likely to be a Cu(Ti)-O mixed oxide at this interface. We discuss the nature of this Cu(Ti)-O interface and interpret its role on the CO oxidation reaction.

  18. Ethylene polymerization in supercritical carbon dioxide with binuclear nickel(II) catalysts

    OpenAIRE

    Guironnet, Damien; Friedberger, Tobias; Mecking, Stefan

    2009-01-01

    A series of new, highly fluorinated neutral (kappa(2)-N,O) chelated Ni(II) binuclear complexes based on salicylaldimines bridged in p-position of the N-aryl group were prepared. The complexes are single-component catalyst precursors for ethylene polymerization in supercritical carbon dioxide and toluene. Solubility of the catalyst precursors in supercritical carbon dioxide is effected by a large number of up to 18 trifluoromethyl groups per molecule. Semicrystalline polyethylene with a low de...

  19. Study on the Reaction Mechanism for Carbon Dioxide Reforming of Methane over supported Nickel Catalyst

    Institute of Scientific and Technical Information of China (English)

    Ling QIAN; Zi Feng YAN

    2003-01-01

    The adsorption and dissociation of methane and carbon dioxide for reforming on nickelcatalyst were extensively investigated by TPSR and TPD experiments. It showed that thedecomposition of methane results in the formation of at least three kinds of surface carbon specieson supported nickel catalyst, while CO2 adsorbed on the catalyst weakly and only existed in onekind of adsorption state. Then the mechanism of interaction between the species dissociatedfrom CH4 and CO2 during reforming was proposed.

  20. CoxC encased in carbon nanotubes: an efficient oxygen reduction catalyst under both acidic and alkaline conditions.

    Science.gov (United States)

    Chen, Lisong; Cui, Xiangzhi; Wang, Qingsong; Zhang, Xiaohua; Wan, Gang; Cui, Fangming; Wei, Chenyang; Shi, Jianlin

    2015-12-21

    The design of a non-precious metal oxygen reduction reaction (ORR) catalyst of high activity and long durability in acidic electrolyte is of great importance for the development and commercialization of low-temperature fuel cells, which remains a great challenge to date. Here, we demonstrate a facile, scalable protocol for the controlled synthesis of CoxC encapsulated in carbon nanotubes as a novel kind of efficient electrochemical oxygen reduction reaction (ORR) catalyst. The synthesized CoxC/carbon nanotube features a high BET surface area, large pore volume and high graphitic content, which greatly favors enhanced ORR properties. The resultant composite electro-catalyst shows high ORR activity which is comparable with that of 20 wt% Pt/C in 0.1 M KOH electrolyte. More importantly, it also exhibits a high ORR activity in 0.1 M HClO4 with a near-complete 4e pathway. More attractively, compared to the most investigated FexC, CoxC as the proposed main catalytically active center shows much enhanced activity in acidic electrolyte, which will pave the way towards the rational design of an advanced electro-catalyst for an efficient ORR process especially under acidic conditions. Moreover, a fuel cell using the synthesized CoxC/carbon nanotube as a cathode catalyst showed a large open-circuit potential, high output power density and long durability, which make it a promising alternative to Pt/C as a non-precious metal ORR catalyst in proton exchange membrane fuel cells.

  1. Tungsten Promoted Ni/Al2O3 Catalysts for Carbon Dioxide Reforming of Methane to Synthesis Gas

    Institute of Scientific and Technical Information of China (English)

    XIAO Tian-cun; Thomas Suhartanto; Andrew P. E. York; Malcolm L. H. Green

    2004-01-01

    A series of tungsten promoted alumina supported nickel catalysts has been prepared for the carbon dioxide reforming of methane to synthesis gas. The catalysts have been characterized by means of XRD, TEM,and Laser Raman spectroscopy. It is shown that the addition of tungsten to the nickel catalyst can stabilize the catalyst and increase the resistance to carbon deposition. Adding a suitable amount of tungsten can also increase the catalyst activity to be close to that of supported noble metal catalysts. The carburisation of the tungsten modified nickel catalyst decreases the catalyst activity at lower reaction temperatures(<1123K),but has no effect on the catalyst performance at higher reaction temperatures. The alumina supported nickel catalyst modified by 0. 67 % (mass fraction)WOs has the equivalent equilibrium constant of the dry reforming reaction to that of alumina supported 5% (mass fraction) Ru at 873 K, and also has a lower activation energy for dry reforming than the latter.

  2. Effect of nitrogen post-doping on a commercial platinum-ruthenium/carbon anode catalyst

    Science.gov (United States)

    Corpuz, April R.; Wood, Kevin N.; Pylypenko, Svitlana; Dameron, Arrelaine A.; Joghee, Prabhuram; Olson, Tim S.; Bender, Guido; Dinh, Huyen N.; Gennett, Thomas; Richards, Ryan M.; O'Hayre, Ryan

    2014-02-01

    This work investigates the effects of after-the-fact chemical modification of a state-of-the-art commercial carbon-supported PtRu catalyst for direct methanol fuel cells (DMFCs). A commercial PtRu/C (JM HiSPEC-10000) catalyst is post-doped with nitrogen by ion-implantation, where "post-doped" denotes nitrogen doping after metal is carbon-supported. Composition and performance of the PtRu/C catalyst post-modified with nitrogen at several dosages are evaluated using X-ray photoelectron spectroscopy (XPS), rotating disk electrode (RDE), and membrane electrode assemblies (MEAs) for DMFC. Overall, implantation at high dosage results in 16% higher electrochemical surface area and enhances performance, specifically in the mass transfer region. Rotating disk electrode (RDE) results show that after 5000 cycles of accelerated durability testing to high potential, the modified catalyst retains 34% more electrochemical surface area (ECSA) than the unmodified catalyst. The benefits of nitrogen post-doping are further substantiated by DMFC durability studies (carried out for 425 h), where the MEA with the modified catalyst exhibits higher surface area and performance stability in comparison to the MEA with unmodified catalyst. These results demonstrate that post-doping of nitrogen in a commercial PtRu/C catalyst is an effective approach, capable of improving the performance of available best-in-class commercial catalysts.

  3. Durability of Carbon Nanofiber (CNF) & Carbon Nanotube (CNT) as Catalyst Support for Proton Exchange Membrane Fuel Cells

    DEFF Research Database (Denmark)

    Andersen, Shuang Ma; Borghei, Maryam; Lund, Peter;

    2013-01-01

    (normally carbon black) is one of the essential degradation mechanisms during cell operation. In this work, durability of Carbon Nanofibers (CNF) & Carbon Nanotubes (CNT) as alternative platinum catalyst supports for Proton Exchange Membrane Fuel Cells (PEMFCs) was assessed. Platinized CNF and CNT using...... a standard polyol method were prepared and fabricated as cathodes of Membrane Electrode Assemblies (MEA) for PEMFC. Both the catalysts as such and the MEAs made out of them were evaluated regarding to thermal and electrochemical stability using traditional carbon black (Vulcan XC72) as a reference. Thermal...... gravimetric analysis (TGA), cyclic voltammetry (CV), polarization curve and impedance spectroscopy were applied on the samples under accelerated stress conditions. The carbon nano-materials demonstrated better stability as support for nano-sized platinum catalyst under PEMFC related operating conditions. Due...

  4. Reactivity of a Carbon-Supported Single-Site Molybdenum Dioxo Catalyst for Biodiesel Synthesis

    Energy Technology Data Exchange (ETDEWEB)

    Mouat, Aidan R.; Lohr, Tracy L.; Wegener, Evan C.; Miller, Jeffrey T.; Delferro, Massimiliano; Stair, Peter C.; Marks, Tobin J.

    2016-08-23

    A single-site molybdenum dioxo catalyst, (Oc)2Mo(=O)2@C, was prepared via direct grafting of MoO2Cl2(dme) (dme = 1,2-dimethoxyethane) on high-surface- area activated carbon. The physicochemical and chemical properties of this catalyst were fully characterized by N2 physisorption, ICP-AES/OES, PXRD, STEM, XPS, XAS, temperature-programmed reduction with H2 (TPR-H2), and temperature-programmed NH3 desorption (TPD-NH3). The single-site nature of the Mo species is corroborated by XPS and TPR-H2 data, and it exhibits the lowest reported MoOx Tmax of reduction reported to date, suggesting a highly reactive MoVI center. (Oc)2Mo(=O)2@C catalyzes the transesterification of a variety of esters and triglycerides with ethanol, exhibiting high activity at moderate temperatures (60-90 °C) and with negligible deactivation. (Oc)2Mo(=O)2@C is resistant to water and can be recycled at least three times with no loss of activity. The transesterification reaction is determined experimentally to be first order in [ethanol] and first order in [Mo] with ΔH = 10.5(8) kcal mol-1 and ΔS = -32(2) eu. The low energy of activation is consistent with the moderate conditions needed to achieve rapid turnover. This highly active carbon-supported single-site molybdenum dioxo species is thus an efficient, robust, and lowcost catalyst with significant potential for transesterification processes.

  5. H{sub 2} production from methane pyrolysis over commercial carbon catalysts: Kinetic and deactivation study

    Energy Technology Data Exchange (ETDEWEB)

    Serrano, D.P.; Botas, J.A. [Chemical and Environmental Technology Department, ESCET, Rey Juan Carlos University, C/Tulipan s/n, 28933 Mostoles (Spain); IMDEA Energia, C/Tulipan s/n, 28933 Mostoles (Spain); Guil-Lopez, R. [Chemical and Environmental Technology Department, ESCET, Rey Juan Carlos University, C/Tulipan s/n, 28933 Mostoles (Spain)

    2009-05-15

    Hydrogen production from catalytic methane decomposition (DeCH{sub 4}) is a simple process to produce high purity hydrogen with no formation of carbon oxides (CO or CO{sub 2}). However, to completely avoid those emissions, the catalyst must not be regenerated. Therefore, it is necessary to use inexpensive catalysts, which show low deactivation during the process. Use of carbon materials as catalysts fulfils these requirements. Methane decomposition catalysed by a number of commercial carbons has been studied in this work using both constant and variable temperature experiments. The results obtained showed that the most active catalyst at short reaction times was activated carbon, but it underwent a fast deactivation due to the deposition of the carbon formed from methane cracking. On the contrary, carbon blacks, and especially the CB-bp sample, present high reaction rates for methane decomposition at both short and long reaction times. Carbon nanotubes exhibit a relatively low activity in spite of containing significant amounts of metals. The initial loss of activity observed with the different catalysts is attributed mainly to the blockage of their micropores due to the deposition of the carbon formed during the reaction. (author)

  6. Synthesis of carbon nanotubes by catalytic pyrolysis method with Feitknecht compound as precursor of NiZnAl catalyst

    Institute of Scientific and Technical Information of China (English)

    Yan Xiaoqi; Liu Quanrun; Zhang Songlin; Zhang Kun; Chen Jiuling; Li Yongdan

    2004-01-01

    Carbon nanotubes are synthesized by catalytic pyrolysis method with a kind of new type catalyst--nickel-zinc-alumina catalyst prepared from Feitknecht compound. Tubular carbon nanotubes, bamboo-shaped carbon naotubes, herringbone carbon nanotubues and branched carbon nanotubes are all found formed at moderate temperature. It is important for the formation of quasi-liquid state of the metal nanoparticles at the tip of carbon naotubes during the growth of carbon nanotubes to lead to different kinds of carbon nanotubes. It is likely that the addition of zinc make the activity of nickel catalyst after calcinations and reduction changed strangely.

  7. Influence of Supports on Catalytic Performance and Carbon Deposition of Palladium Catalyst for Methane Partial Oxidation

    Institute of Scientific and Technical Information of China (English)

    Shi Fangli; Shen Meiqing; Fei Yanan; Wang Jun; Weng Duan

    2007-01-01

    The catalytic performance of methane partial oxidation was investigated on Pd/CeO2-ZrO2 and Pd/α-Al2O3 catalysts. The catalysts were characterized by XRD, Raman spectra, and TG-DTA techniques. The results show that CeO2-ZrO2 support is more advantageous for the catalytic activity and stability of catalysts compared to α-Al2O3. TG-DTA and Raman spectra results indicated that carbon deposited on the catalysts was in the form of graphite, which is the main reason for the deactivation of catalysts after a 24-hour reaction. Moreover, CeO2-ZrO2 had positive effect on inhibiting carbon deposition.

  8. Enhancement of Nitrite Reduction Kinetics on Electrospun Pd-Carbon Nanomaterial Catalysts for Water Purification.

    Science.gov (United States)

    Ye, Tao; Durkin, David P; Hu, Maocong; Wang, Xianqin; Banek, Nathan A; Wagner, Michael J; Shuai, Danmeng

    2016-07-20

    We report a facile synthesis method for carbon nanofiber (CNF) supported Pd catalysts via one-pot electrospinning and their application for nitrite hydrogenation. A mixture of Pd acetylacetonate (Pd(acac)2), polyacrylonitrile (PAN), and nonfunctionalized multiwalled carbon nanotubes (MWCNTs) was electrospun and thermally treated to produce Pd/CNF-MWCNT catalysts. The addition of MWCNTs with a mass loading of 1.0-2.5 wt % (to PAN) significantly improved nitrite reduction activity compared to the catalyst without MWCNT addition. The results of CO chemisorption confirmed that the addition of MWCNTs increased Pd exposure on CNFs and hence improved catalytic activity.

  9. Enhancement of Nitrite Reduction Kinetics on Electrospun Pd-Carbon Nanomaterial Catalysts for Water Purification.

    Science.gov (United States)

    Ye, Tao; Durkin, David P; Hu, Maocong; Wang, Xianqin; Banek, Nathan A; Wagner, Michael J; Shuai, Danmeng

    2016-07-20

    We report a facile synthesis method for carbon nanofiber (CNF) supported Pd catalysts via one-pot electrospinning and their application for nitrite hydrogenation. A mixture of Pd acetylacetonate (Pd(acac)2), polyacrylonitrile (PAN), and nonfunctionalized multiwalled carbon nanotubes (MWCNTs) was electrospun and thermally treated to produce Pd/CNF-MWCNT catalysts. The addition of MWCNTs with a mass loading of 1.0-2.5 wt % (to PAN) significantly improved nitrite reduction activity compared to the catalyst without MWCNT addition. The results of CO chemisorption confirmed that the addition of MWCNTs increased Pd exposure on CNFs and hence improved catalytic activity. PMID:27387354

  10. Effects of catalyst precursors on carbon nanowires by using ethanol catalytic combustion technique

    Institute of Scientific and Technical Information of China (English)

    CHENG Jin; ZOU Xiao-ping; LI Fei; ZHANG Hong-dan; REN Peng-fei

    2006-01-01

    Iron nitrate,nickel nitrate and cobalt nitrate were used as catalyst precursors to study their effects on carbon nanowires synthesized by ethanol catalytic combustion (ECC) process. The as-grown carbon nanowires were characterized by means of scanning electron microscopy,transmission electron microscopy and Raman spectroscopy. The results show that relatively uniform nanowires will be formed when the catalyst precursor is iron nitrate:while helical structure or disordered structure will be formed when the catalyst precursor is nickel nitrate or cobalt nitrate.

  11. Nanocrystalline MgO supported nickel-based bimetallic catalysts for carbon dioxide reforming of methane

    Energy Technology Data Exchange (ETDEWEB)

    Meshkani, Fereshteh [Catalyst and Advanced Materials Research Laboratory, Chemical Engineering Department, Faculty of Engineering, University of Kashan, Kashan (Iran); Rezaei, Mehran [Catalyst and Advanced Materials Research Laboratory, Chemical Engineering Department, Faculty of Engineering, University of Kashan, Kashan (Iran); Institute of Nanoscience and Nanotechnology, University of Kashan, Kashan (Iran)

    2010-10-15

    Nanocrystalline magnesium oxide with high surface area and plate-like shape was employed as catalyst support for preparation of nickel-based bimetallic catalysts in methane reforming with carbon dioxide. The prepared samples were characterized by X-ray diffraction (XRD), N{sub 2} adsorption (BET), Temperature programmed oxidation and desorption (TPO-TPD), Thermal gravimetric and differential thermal gravimetric (TGA-DTG), H{sub 2} chemisorption and Transmission and electron microscopies (TEM and SEM) analyses. CO{sub 2}-TPD data showed the high CO{sub 2} adsorption capacity of catalysts which improves the resistance of catalysts against the carbon formation. The H{sub 2} chemisorption results also indicated that the addition of Pt to nickel catalyst improved the nickel dispersion. The obtained results revealed that the prepared catalysts showed a high activity and stability during the reaction with a low amount of deposited carbon. Addition of Pt to nickel catalyst improved both the activity and resistivity against carbon formation. (author)

  12. Oxidation catalyst

    Science.gov (United States)

    Ceyer, Sylvia T.; Lahr, David L.

    2010-11-09

    The present invention generally relates to catalyst systems and methods for oxidation of carbon monoxide. The invention involves catalyst compositions which may be advantageously altered by, for example, modification of the catalyst surface to enhance catalyst performance. Catalyst systems of the present invention may be capable of performing the oxidation of carbon monoxide at relatively lower temperatures (e.g., 200 K and below) and at relatively higher reaction rates than known catalysts. Additionally, catalyst systems disclosed herein may be substantially lower in cost than current commercial catalysts. Such catalyst systems may be useful in, for example, catalytic converters, fuel cells, sensors, and the like.

  13. Nitrogen-doped carbon-supported cobalt-iron oxygen reduction catalyst

    Science.gov (United States)

    Zelenay, Piotr; Wu, Gang

    2014-04-29

    A Fe--Co hybrid catalyst for oxygen reaction reduction was prepared by a two part process. The first part involves reacting an ethyleneamine with a cobalt-containing precursor to form a cobalt-containing complex, combining the cobalt-containing complex with an electroconductive carbon supporting material, heating the cobalt-containing complex and carbon supporting material under conditions suitable to convert the cobalt-containing complex and carbon supporting material into a cobalt-containing catalyst support. The second part of the process involves polymerizing an aniline in the presence of said cobalt-containing catalyst support and an iron-containing compound under conditions suitable to form a supported, cobalt-containing, iron-bound polyaniline species, and subjecting said supported, cobalt-containing, iron bound polyaniline species to conditions suitable for producing a Fe--Co hybrid catalyst.

  14. Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene

    Science.gov (United States)

    Mistry, Hemma; Varela, Ana Sofia; Bonifacio, Cecile S.; Zegkinoglou, Ioannis; Sinev, Ilya; Choi, Yong-Wook; Kisslinger, Kim; Stach, Eric A.; Yang, Judith C.; Strasser, Peter; Cuenya, Beatriz Roldan

    2016-06-01

    There is an urgent need to develop technologies that use renewable energy to convert waste products such as carbon dioxide into hydrocarbon fuels. Carbon dioxide can be electrochemically reduced to hydrocarbons over copper catalysts, although higher efficiency is required. We have developed oxidized copper catalysts displaying lower overpotentials for carbon dioxide electroreduction and record selectivity towards ethylene (60%) through facile and tunable plasma treatments. Herein we provide insight into the improved performance of these catalysts by combining electrochemical measurements with microscopic and spectroscopic characterization techniques. Operando X-ray absorption spectroscopy and cross-sectional scanning transmission electron microscopy show that copper oxides are surprisingly resistant to reduction and copper+ species remain on the surface during the reaction. Our results demonstrate that the roughness of oxide-derived copper catalysts plays only a partial role in determining the catalytic performance, while the presence of copper+ is key for lowering the onset potential and enhancing ethylene selectivity.

  15. Physicochemical investigations of carbon nanofiber supported Cu/ZrO{sub 2} catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Din, Israf Ud, E-mail: drisraf@yahoo.com, E-mail: maizats@petronas.com.my; Shaharun, Maizatul S., E-mail: drisraf@yahoo.com, E-mail: maizats@petronas.com.my [Department of Fundamental and Applied Sciences, Universiti Teknologi PETRONAS (Malaysia); Subbarao, Duvvuri, E-mail: duvvuri-subbarao@petronas.com.my [Department of Chemical Engineering, Universiti Teknologi PETRONAS (Malaysia); Naeem, A., E-mail: naeeem64@yahoo.com [National Centre of Excellence in Physical Chemistry, University of Peshawar (Pakistan)

    2014-10-24

    Zirconia-promoted copper/carbon nanofiber catalysts (Cu‐ZrO{sub 2}/CNF) were prepared by the sequential deposition precipitation method. The Herringbone type of carbon nanofiber GNF-100 (Graphite nanofiber) was used as a catalyst support. Carbon nanofiber was oxidized to (CNF-O) with 5% and 65 % concentration of nitric acid (HNO{sub 3}). The CNF activated with 5% HNO{sub 3} produced higher surface area which is 155 m{sup 2}/g. The catalyst was characterized by X-ray Diffraction (XRD), Fourier Transform Infra-Red (FTIR) and N{sub 2} adsorption-desorption. The results showed that increase of HNO{sub 3} concentration reduced the surface area and porosity of the catalyst.

  16. Conversion of biomass-derived sorbitol to glycols over carbon-materials supported Ru-based catalysts

    Science.gov (United States)

    Guo, Xingcui; Guan, Jing; Li, Bin; Wang, Xicheng; Mu, Xindong; Liu, Huizhou

    2015-11-01

    Ruthenium (Ru) supported on activated carbon (AC) and carbon nanotubes (CNTs) was carried out in the hydrogenolysis of sorbitol to ethylene glycol (EG) and 1,2-propanediol (1,2-PD) under the promotion of tungsten (WOx) species and different bases. Their catalytic activities and glycols selectivities strongly depended on the support properties and location of Ru on CNTs, owning to the altered metal-support interactions and electronic state of ruthenium. Ru located outside of the tubes showed excellent catalytic performance than those encapsulated inside the nanotubes. Additionally, the introduction of WOx into Ru/CNTs significantly improved the hydrogenolysis activities, and a complete conversion of sorbitol with up to 60.2% 1,2-PD and EG yields was obtained on RuWOx/CNTs catalyst upon addition of Ca(OH)2. Stability study showed that this catalyst was highly stable against leaching and poisoning and could be recycled several times.

  17. Nickel-carbon nanocomposites prepared using castor oil as precursor: A novel catalyst for ethanol steam reforming

    Science.gov (United States)

    Carreño, Neftalí L. V.; Garcia, Irene T. S.; Raubach, Cristiane W.; Krolow, Mateus; Santos, Cláudia C. G.; Probst, Luiz F. D.; Fajardo, Humberto V.

    A novel and simple method to prepare nickel-based catalysts for ethanol steam reforming is proposed. The present method was developed using castor oil as a precursor. The results clarify that the nickel-carbon (Ni/C) catalyst has a high activity for ethanol steam reforming. It was observed that the catalytic behavior could be modified according to the experimental conditions employed. Moreover, it is interesting to note that the increase in the catalytic activity of the Ni/C nanocomposite over time, at 500 and 600 °C of reaction temperature, may be associated with the formation of filamentous carbon. The preliminary results indicate that the novel methodology used, led to the obtainment of materials with important properties that can be extended to applications in different catalytic process.

  18. Molybdosphoric Acid Mixed with Titania Used as a Catalyst to Synthesize Diphenyl Carbonate via Transesterification of Dimethyl Carbonate and Phenol

    Institute of Scientific and Technical Information of China (English)

    Tong Chen; Huajun Han; Zhiping Du; Jie Yao; Gongying Wang; Dachuan Shi; Desheng Zhang; Zhiming Chen

    2006-01-01

    The 12-molybdosphoric acid mixed with titania (MPA-TiO2) was found to be a novel and efficient catalyst for the synthesis of diphenyl carbonate (DPC) via transesterification of dimethyl carbonate (DMC) and phenol. The X-ray diffraction (XRD) and infrared (IR) techniques were employed to characterize the prepared catalysts. The effect of the weight ratio of the 12-molybdosphoric acid to titania on the transesterification was investigated. A 13.1% yield of DPC and an 11.6% yield of methyl phenyl carbonate (MPC) were obtained over MPA-TiO2 with the weight ratio of MPA to TiO2 as 5:1.

  19. Development of Pd and Pd-Co catalysts supported on multi-walled carbon nanotubes for formic acid oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Morales-Acosta, D.; Godinez, Luis A.; Rodriguez, H.G.; Arriaga, L.G. [Centro de Investigacion y Desarrollo Tecnologico en Electroquimica, Parque Tecnologico Queretaro, Sanfandila, Pedro Escobedo, C.P. 76703 Queretaro (Mexico); Ledesma-Garcia, J. [Division de Investigacion y Posgrado, Facultad de Ingenieria, Universidad Autonoma de Queretaro, Cerro de las Campanas S/N, C.P. 76010, Queretaro, Qro. (Mexico); Alvarez-Contreras, L. [Centro de Investigacion en Materiales Avanzados S. C., Complejo Industrial Chihuahua, C.P. 31109, Chihuahua, Chih. (Mexico)

    2010-01-15

    Pd-Co and Pd catalysts were prepared by the impregnation synthesis method at low temperature on multi-walled carbon nanotubes (MWCNTs). The nanotubes were synthesized by spray pyrolysis technique. Both catalysts were obtained with high homogeneous distribution and particle size around 4 nm. The morphology, composition and electrocatalytic properties were investigated by transmission electron microscopy, scanning electron microscopy-energy dispersive X-ray analysis, X-ray diffraction and electrochemical measurements, respectively. The electrocatalytic activity of Pd and PdCo/MWCNTs catalysts was investigated in terms of formic acid electrooxidation at low concentration in H{sub 2}SO{sub 4} aqueous solution. The results obtained from voltamperometric studies showed that the current density achieved with the PdCo/MWCNTs catalyst is 3 times higher than that reached with the Pd/MWCNTs catalyst. The onset potential for formic acid electrooxidation on PdCo/MWCNTs electrocatalyst showed a negative shift ca. 50 mV compared with Pd/MWCNTs. (author)

  20. HDO of guaiacol over NiMo catalyst supported on activated carbon derived from castor de-oiled cake

    Directory of Open Access Journals (Sweden)

    Viviana Ospina

    2015-08-01

    Full Text Available Physical and chemical activation methods were used to prepare two different activated carbons (ACs from castor de-oiled cake. H2O/CO2 mixture was used as the physical activating agent, and for chemical activation potassium carbonate (K2CO3 was used. For both materials, textural and chemical properties were characterized by N2 adsorption–desorption isotherms, thermogravimetric analysis (TGA, Fourier Transform Infrared Spectroscopy (FTIR, thermal programmed reduction (TPR, X-ray fluorescence (XRF, and scanning electron microscopy (SEM. The ACs were used as supports for NiMo sulfide catalysts, which were prepared by wetness impregnation and in-situ sulfided for the hydrodeoxygenation (HDO of guaiacol (GUA as a model compound of bio-oil. The HDO reaction was carried out in a typical batch reactor at 5 MPa of H2 and 350 °C. Under the same test conditions, commercial catalysts were also tested in the reaction. Although the commercial catalysts displayed higher GUA conversion, the prepared catalysts showed higher activity and non-oxygenated and saturated products yield. 

  1. Nitrogen-Doped Carbon Nanoparticle-Carbon Nanofiber Composite as an Efficient Metal-Free Cathode Catalyst for Oxygen Reduction Reaction.

    Science.gov (United States)

    Panomsuwan, Gasidit; Saito, Nagahiro; Ishizaki, Takahiro

    2016-03-23

    Metal-free nitrogen-doped carbon materials are currently considered at the forefront of potential alternative cathode catalysts for the oxygen reduction reaction (ORR) in fuel cell technology. Despite numerous efforts in this area over the past decade, rational design and development of a new catalyst system based on nitrogen-doped carbon materials via an innovative approach still present intriguing challenges in ORR catalysis research. Herein, a new kind of nitrogen-doped carbon nanoparticle-carbon nanofiber (NCNP-CNF) composite with highly efficient and stable ORR catalytic activity has been developed via a new approach assisted by a solution plasma process. The integration of NCNPs and CNFs by the solution plasma process can lead to a unique morphological feature and modify physicochemical properties. The NCNP-CNF composite exhibits a significantly enhanced ORR activity through a dominant four-electron pathway in an alkaline solution. The enhancement in ORR activity of NCNP-CNF composite can be attributed to the synergistic effects of good electron transport from highly graphitized CNFs as well as abundance of exposed catalytic sites and meso/macroporosity from NCNPs. More importantly, NCNP-CNF composite reveals excellent long-term durability and high tolerance to methanol crossover compared with those of a commercial 20 wt % supported on Vulcan XC-72. We expect that NCNP-CNF composite prepared by this synthetic approach can be a promising metal-free cathode catalyst candidate for ORR in fuel cells and metal-air batteries. PMID:26908214

  2. Oxidative steam reforming of ethanol over carbon nanofiber supported Co catalysts

    NARCIS (Netherlands)

    da Silva, A.L.M.; Mattos, L.V.; den Breejen, J.P.; Bitter, J.H.; de Jong, K.P.; Noronha, F.B.

    2011-01-01

    The effect of the cobalt particle size in the ethanol oxidative steam reforming reaction for hydrogen production was investigated using cobalt on carbon nanofiber catalysts. The smallest (4 nm) were quite stable during OSR reaction but significant carbon formation was detected.

  3. Studies on Co-based catalysts supported on modified carbon substrates for PEMFC cathodes

    Energy Technology Data Exchange (ETDEWEB)

    Subramanian, Nalini P.; Kumaraguru, Swaminatha P.; Colon-Mercado, Hector; Popov, Branko N. [Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208 (United States); Kim, Hansung [Department of Chemical Engineering Yonsei University, Seoul (Korea, Republic of); Black, Timothy; Chen, Donna A. [Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 (United States)

    2006-06-19

    Cobalt based non-precious metal catalysts were prepared by supporting cobalt-ethylene diamine complex on carbon followed by a heat treatment at elevated temperatures (800{sup o}C). Surface oxygen groups on carbon were introduced with HNO{sub 3} oxidation. Co catalysts supported on oxidized carbon showed improved activity and selectivity towards four-electron reduction of molecular oxygen. Quinone groups introduced by nitric acid treatment, in addition to increasing the dispersion of the chelate complexes, play a role in forming the active site for oxygen reduction. (author)

  4. Transesterification of Ethylene Carbonate with Dimethyl Terephthalate over Various Metal Acetate Catalysts

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    The reaction between ethylene carbonate and dimethyl terephthalate was carried out for the simultaneous synthesis of dimethyl carbonate and poly( ethylene terephthalate). This reaction is an excellent chemical process that is environmentally friendly and produces no poisonous substance. The metal acetate catalysts used for this reaction are discussed in detail. Lithium acetate dihydrate was found to be a novel and efficient catalyst for this reaction. Compared with other metal acetates, lithium acetate dihydrate can attain a maximum catalytic activity at a lower concentration.When the reaction was carried out under the following conditions: the reaction temperature from 230 to 250 ℃, molar ratio of ethylene carbonate(EC) to dimethyl terephthalate(DMT) 3: 1, reaction time 3 h, and a catalyst amount of 0. 4% (molar fraction to DMT), the yield of dimethyl carbonate(DMC) was 79. 1%.

  5. In-situ observations of catalyst dynamics during surface-bound carbon nanotube nucleation

    DEFF Research Database (Denmark)

    Hofmann, S; Sharma, R; Du, G;

    2007-01-01

    We present atomic-scale, video-rate environmental transmission electron microscopy and in situ time-resolved X-ray photoelectron spectroscopy of surface-bound catalytic chemical vapor deposition of single-walled carbon nanotubes and nanofibers. We observe that transition metal catalyst...... nanoparticles on SiOx support show crystalline lattice fringe contrast and high deformability before and during nanotube formation. A single-walled carbon nanotube nucleates by lift-off of a carbon cap. Cap stabilization and nanotube growth involve the dynamic reshaping of the catalyst nanocrystal itself....... For a carbon nanofiber, the graphene layer stacking is determined by the successive elongation and contraction of the catalyst nanoparticle at its tip....

  6. Research of special carbon nanobeads supported Pt catalyst for fuel cell through high temperature pyrolysis and deposition from novel phthalocyanine

    Institute of Scientific and Technical Information of China (English)

    GUO Yanchuan; YUE Jun; PAN Zhongxiao; XU Haitao; ZHANG Bing; HAN Fengmei; CHEN Lijuan; PENG Bixian; XIE Wenwei; QIAN Haisheng; YAN Tiantang

    2004-01-01

    The carbon nanobeads were prepared through high temperature pyrolysis and deposition from phthaiocyanine. After surface's functionalization treatment of the carbon beads, the carbon nanobeads supported Pt catalyst was produced. The Pt/C catalyst was characterized by SEM,TEM, Raman spectrum, EDS and XRD methods. Combining the carbonaceous paper spreaded up with the catalyst with Nafion membrane, we made MEA electrode. The discharge curves indicated that this carbon nanobeads supported Pt is a good fuel cell catalyst with excellent performance, high activity and sign of a long-time life.

  7. Combination of carbon nitride and carbon nanotubes: synergistic catalysts for energy conversion.

    Science.gov (United States)

    Gong, Yutong; Wang, Jing; Wei, Zhongzhe; Zhang, Pengfei; Li, Haoran; Wang, Yong

    2014-08-01

    Due to their versatile features and environmental friendliness, functionalized carbon materials show great potential in practical applications, especially in energy conversion. Developing carbon composites with properties that can be modulated by simply changing the ratio of the original materials is an intriguing synthetic strategy. Here, we took cyanamide and multiwalled carbon nanotubes as precursors and introduced a facile method to fabricate a series of graphitic carbon nitride/carbon nanotubes (g-C3 N4 /CNTs) composites. These composites demonstrated different practical applications with different weight ratios of the components, that is, they showed synergistic effects in optoelectronic conversion when g-C3 N4 was the main ingredient and in oxygen reduction reaction (ORR) when CNTs dominated the composites. Our experiments indicated that the high electrical conductivity of carbon nanotubes promoted the transmission of the charges in both cases.

  8. Ultrafine Cobalt Catalysts on Covalent Carbon Nitride Frameworks for Oxygenic Photosynthesis.

    Science.gov (United States)

    Zhang, Guigang; Zang, Shaohong; Lin, Lihua; Lan, Zhi-An; Li, Guosheng; Wang, Xinchen

    2016-01-27

    The rational cooperation of sustainable catalysts with suitable light-harvesting semiconductors to fabricate photosynthetic device/machinery has been regarded as an ideal technique to alleviate the current worldwide energy and environmental issues. Cobalt based species (e.g., Co-Pi, Co3O4, and Co-cubene) have attracted particular attentions because they are earth-abundant, cost-acceptable, and more importantly, it shows comparable water oxidation activities to the noble metal based catalysts (e.g., RuO2, IrO2). In this contribution, we compared two general cocatalysts modification strategies, based on the surface depositing and bulk doping of ultrafine cobalt species into the sustainable graphitic carbon nitride (g-C3N4) polymer networks for oxygenic photosynthesis by splitting water into oxygen, electrons, and protons. The chemical backbone of g-C3N4 does not alter after both engineering modifications; however, in comparison with the bulk doping, the optical and electronic properties of the surface depositing samples are efficiently promoted, and the photocatalytic water oxidation activities are increased owing to much more exposed active sites, reduced overpotential for oxygen evolution and the accelerated interface charge mobility. This paper underlines the advantage of surface engineering to establish efficient advanced polymeric composites for water oxidation, and it opens new insights into the architectural design of binary hybrid photocatalysts with high reactivity and further utilizations in the fields of energy and environment.

  9. Carbon Nanotubes for Thin Film Transistor: Fabrication, Properties, and Applications

    Directory of Open Access Journals (Sweden)

    Yucui Wu

    2013-01-01

    Full Text Available We review the present status of single-walled carbon nanotubes (SWCNTs for their production and purification technologies, as well as the fabrication and properties of single-walled carbon nanotube thin film transistors (SWCNT-TFTs. The most popular SWCNT growth method is chemical vapor deposition (CVD, including plasma-enhanced chemical vapor deposition (PECVD, floating catalyst chemical vapor deposition (FCCVD, and thermal CVD. Carbon nanotubes (CNTs used to fabricate thin film transistors are sorted by electrical breakdown, density gradient ultracentrifugation, or gel-based separation. The technologies of applying CNT random networks to work as the channels of SWCNT-TFTs are also reviewed. Excellent work from global researchers has been benchmarked and analyzed. The unique properties of SWCNT-TFTs have been reviewed. Besides, the promising applications of SWCNT-TFTs have been explored. Finally, the key issues to be solved in future have been summarized.

  10. Low-temperature SCR of NOx with NH3 over carbon-ceramic supported catalysts

    International Nuclear Information System (INIS)

    A new method for preparing vanadium oxide supported on carbon-ceramic cellular monoliths is described. This includes a support oxidation step with HNO3, followed by ionic exchange with a NaOH solution, equilibrium adsorption impregnation of VO2+ and thermal treatment. As a result an active catalyst for low-temperature selective catalytic reduction (SCR) reaction is obtained. The V-catalyst is more resistant to SO2 poisoning than the previously developed Mn-catalyst. Inhibition by water is reversible for both types of catalysts. Testing of the vanadium catalyst after subjecting it to the outlet gas stream of a power plant shows fast deactivation until constant residual activity is reached. Deactivation seems to be caused by arsenic poisoning and the formation of superficial sulphates

  11. Photo-promoted carbonylation of chloroalkanes with carbon monoxide by non-precious metal catalysts

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    The photo-promoted carbonylation of chloroalkanes with carbon monoxide was carried out under ambient conditions with copper and cadmium salts catalysts. The results indicated that the corresponding esters were produced with three salt catalysts, i.e.CuBr2, CuCl2 and CdI2. Among these catalysts, CdI2 was the most efficient in terms of ester yield and selectivity, particularly, 60% yield and 75% selectivity in the carbonylation of chlorocyclohexane were achieved. Furthermore, the yield and selectivity of the ester can be improved greatly by adding tri-n-butylamine in the CuBr2 and CuCl2 catalyst systems. On the other hand, the additive. As a result, we suggest that iodide ion plays an important role in the catalyst system of the cadmium salts.(C) 2007 Ying Ping Jia. Published by Elsevier B.V. on behalf of Chinese Chemical Society. All rights reserved.

  12. Particle size effects in Fischer-Tropsch synthesis by Co catalyst supported on carbon nanotubes

    Institute of Scientific and Technical Information of China (English)

    Ali Nakhaei Pour; Elham Hosaini; Mohammad Izadyar; Mohammad Reza Housaindokht

    2015-01-01

    The effect of Co particle size on the Fischer-Tropsch synthesis (FTS) activity of carbon nanotube (CNT)-supported Co catalysts was investigated. Microemulsion (using water-to-surfactant molar ratios of 2 to12) and impregnation techniques were used to prepare catalysts with different Co particle sizes. Kinetic studies were performed to understand the effect of Co particle size on catalytic activity. Size-dependent kinetic parameters were developed using a thermodynamic method, to evaluate the structural sensitivity of the CNT-supported Co catalysts. The size-independent FTS reaction rate constant and size-independent adsorption parameter increased with increasing reac-tion temperature. The Polani parameter also depended on catalyst particle size, because of changes in the catalyst surface coverage.

  13. Role of the catalyst in the growth of single-wall carbon nanotubes.

    Science.gov (United States)

    Balbuena, Perla B; Zhao, Jin; Huang, Shiping; Wang, Yixuan; Sakulchaicharoen, Nataphan; Resasco, Daniel E

    2006-05-01

    Classical molecular dynamics simulations are carried out to analyze the physical state of the catalyst, and the growth of single-wall carbon nanotubes under typical temperature and pressure conditions of their experimental synthesis, emphasizing the role of the catalyst/substrate interactions. It is found that a strong cluster/substrate interaction increases the cluster melting point, modifying the initial stages of carbon dissolution and precipitation on the cluster surface. Experiments performed on model Co-Mo catalysts clearly illustrate the existence of an initial period where the catalyst is formed and no nanotube growth is observed. To quantify the nature of the Co-Mo2C interaction, quantum density functional theory is applied to characterize structural and energetic features of small Co clusters deposited on a (001) Mo2C surface, revealing a strong attachment of Co-clusters to the Mo2C surface, which may increase the melting point of the cluster and prevent cluster sintering.

  14. Nanoscale zirconia as a nonmetallic catalyst for graphitization of carbon and growth of single- and multiwall carbon nanotubes.

    Science.gov (United States)

    Steiner, Stephen A; Baumann, Theodore F; Bayer, Bernhard C; Blume, Raoul; Worsley, Marcus A; MoberlyChan, Warren J; Shaw, Elisabeth L; Schlögl, Robert; Hart, A John; Hofmann, Stephan; Wardle, Brian L

    2009-09-01

    We report that nanoparticulate zirconia (ZrO(2)) catalyzes both growth of single-wall and multiwall carbon nanotubes (CNTs) by thermal chemical vapor deposition (CVD) and graphitization of solid amorphous carbon. We observe that silica-, silicon nitride-, and alumina-supported zirconia on silicon nucleates single- and multiwall carbon nanotubes upon exposure to hydrocarbons at moderate temperatures (750 degrees C). High-pressure, time-resolved X-ray photoelectron spectroscopy (XPS) of these substrates during carbon nanotube nucleation and growth shows that the zirconia catalyst neither reduces to a metal nor forms a carbide. Point-localized energy-dispersive X-ray spectroscopy (EDAX) using scanning transmission electron microscopy (STEM) confirms catalyst nanoparticles attached to CNTs are zirconia. We also observe that carbon aerogels prepared through pyrolysis of a Zr(IV)-containing resorcinol-formaldehyde polymer aerogel precursor at 800 degrees C contain fullerenic cage structures absent in undoped carbon aerogels. Zirconia nanoparticles embedded in these carbon aerogels are further observed to act as nucleation sites for multiwall carbon nanotube growth upon exposure to hydrocarbons at CVD growth temperatures. Our study unambiguously demonstrates that a nonmetallic catalyst can catalyze CNT growth by thermal CVD while remaining in an oxidized state and provides new insight into the interactions between nanoparticulate metal oxides and carbon at elevated temperatures. PMID:19663436

  15. Effect of Electric Discharge on Properties of Nano-Particulate Catalyst for Plasma-Catalysis.

    Science.gov (United States)

    Lee, Chung Jun; Kim, Jip; Kim, Taegyu

    2016-02-01

    Heterogeneous catalytic processes have been used to produce hydrogen from hydrocarbons. However, high reforming temperature caused serious catalyst deteriorations and low energy efficiency. Recently, a plasma-catalyst hybrid process was used to reduce the reforming temperature and to improve the stability and durability of reforming catalysts. Effect of electric discharges on properties of nanoparticulate catalysts for plasma-catalysis was investigated in the present study. Catalyst-bed porosity was varied by packing catalyst beads with the different size in a reactor. Discharge power and onset voltage of the plasma were measured as the catalyst-bed porosity was varied. The effect of discharge voltage, frequency and voltage waveforms such as the sine, pulse and square was investigated. We found that the optimal porosity of the catalyst-bed exists to maximize the electric discharge. At a low porosity, the electric discharge was unstable to be sustained because the space between catalysts got narrow nearly close to the sheath region. On the other hand, at a high porosity, the electric discharge became weak because the plasma was not sufficient to interact with the surface of catalysts. The discharge power increased as the discharge voltage and frequency increased. The square waveform was more efficient than the sine and pulse one. At a high porosity, however, the effect of the voltage waveform was not considerable because the space between catalysts was too large for plasma to interact with the surface of catalysts.

  16. Direct fabrication of Pt-supported porous carbon catalyst for fuel cell

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, D.Y.; Wang, G.; Konstantinov, K. [Wollongong Univ., NSW (Australia). Inst. for Superconducting and Electronic Materials; Ma, Z.F.; Liub, H.K. [Shanghai Jiaotong Univ., Shanghai (China). Dept. of Chemical Engineering

    2006-07-01

    Platinum (Pt) based electrocatalysts are generally used in proton exchange membrane fuel cells (PEMFC) and in direct alcohol fuel cells (DAFC) operating at relatively low temperature. Wet impregnation techniques and chemical reduction of the metal precursors are the conventional preparation methods for these electrocatalysts. These conventional synthesis methods are based on impregnation-reduction, microemulsions, sonochemistry, and microwave irradiation. However, Pt-supported carbon catalysts cannot be prepared by such methods due to the very long time needed for the synthesis of carbon. In addition, post-fabrication steps must be taken, such as surface modification of carbon and metal supporting. For these reasons, this study presented a new fabrication method for producing Pt-carbon catalysts directly by a Pt-embedded template. The new method provides a time saving route for the preparation of a Pt catalyst supported on a mesoporous carbon. In this study, Pt-supported porous carbon was prepared using the carbon xerogel method. In particular, a platinum salt was dissolved in an aqueous solution of carbon xerogel precursor and reduced under 5 per cent hydrogen/argon gas along with carbonization. Images from a scanning electron microscope revealed that the nanoscale particle structure of the Pt-embedded carbon electrocatalyst had homogeneously distributed bright particles, likely attributed to Pt. 10 refs.

  17. Hemoglobin-carbon nanotube derived noble-metal-free Fe5C2-based catalyst for highly efficient oxygen reduction reaction.

    Science.gov (United States)

    Vij, Varun; Tiwari, Jitendra N; Lee, Wang-Geun; Yoon, Taeseung; Kim, Kwang S

    2016-02-03

    High performance non-precious cathodic catalysts for oxygen reduction reaction (ORR) are vital for the development of energy materials and devices. Here, we report an noble metal free, Fe5C2 nanoparticles-studded sp(2) carbon supported mesoporous material (CNTHb-700) as cathodic catalyst for ORR, which was prepared by pyrolizing the hybrid adduct of single walled carbon nanotubes (CNT) and lyophilized hemoglobin (Hb) at 700 °C. The catalyst shows onset potentials of 0.92 V in 0.1 M HClO4 and in 0.1 M KOH which are as good as commercial Pt/C catalyst, giving very high current density of 6.34 and 6.69 mA cm(-2) at 0.55 V vs. reversible hydrogen electrode (RHE), respectively. This catalyst has been confirmed to follow 4-electron mechanism for ORR and shows high electrochemical stability in both acidic and basic media. Catalyst CNTHb-700 possesses much higher tolerance towards methanol than the commercial Pt/C catalyst. Highly efficient catalytic properties of CNTHb-700 could lead to fundamental understanding of utilization of biomolecules in ORR and materialization of proton exchange membrane fuel cells for clean energy production.

  18. Hemoglobin-carbon nanotube derived noble-metal-free Fe5C2-based catalyst for highly efficient oxygen reduction reaction

    Science.gov (United States)

    Vij, Varun; Tiwari, Jitendra N.; Lee, Wang-Geun; Yoon, Taeseung; Kim, Kwang S.

    2016-01-01

    High performance non-precious cathodic catalysts for oxygen reduction reaction (ORR) are vital for the development of energy materials and devices. Here, we report an noble metal free, Fe5C2 nanoparticles-studded sp2 carbon supported mesoporous material (CNTHb-700) as cathodic catalyst for ORR, which was prepared by pyrolizing the hybrid adduct of single walled carbon nanotubes (CNT) and lyophilized hemoglobin (Hb) at 700 °C. The catalyst shows onset potentials of 0.92 V in 0.1 M HClO4 and in 0.1 M KOH which are as good as commercial Pt/C catalyst, giving very high current density of 6.34 and 6.69 mA cm−2 at 0.55 V vs. reversible hydrogen electrode (RHE), respectively. This catalyst has been confirmed to follow 4-electron mechanism for ORR and shows high electrochemical stability in both acidic and basic media. Catalyst CNTHb-700 possesses much higher tolerance towards methanol than the commercial Pt/C catalyst. Highly efficient catalytic properties of CNTHb-700 could lead to fundamental understanding of utilization of biomolecules in ORR and materialization of proton exchange membrane fuel cells for clean energy production. PMID:26839148

  19. Hemoglobin-carbon nanotube derived noble-metal-free Fe5C2-based catalyst for highly efficient oxygen reduction reaction

    Science.gov (United States)

    Vij, Varun; Tiwari, Jitendra N.; Lee, Wang-Geun; Yoon, Taeseung; Kim, Kwang S.

    2016-02-01

    High performance non-precious cathodic catalysts for oxygen reduction reaction (ORR) are vital for the development of energy materials and devices. Here, we report an noble metal free, Fe5C2 nanoparticles-studded sp2 carbon supported mesoporous material (CNTHb-700) as cathodic catalyst for ORR, which was prepared by pyrolizing the hybrid adduct of single walled carbon nanotubes (CNT) and lyophilized hemoglobin (Hb) at 700 °C. The catalyst shows onset potentials of 0.92 V in 0.1 M HClO4 and in 0.1 M KOH which are as good as commercial Pt/C catalyst, giving very high current density of 6.34 and 6.69 mA cm-2 at 0.55 V vs. reversible hydrogen electrode (RHE), respectively. This catalyst has been confirmed to follow 4-electron mechanism for ORR and shows high electrochemical stability in both acidic and basic media. Catalyst CNTHb-700 possesses much higher tolerance towards methanol than the commercial Pt/C catalyst. Highly efficient catalytic properties of CNTHb-700 could lead to fundamental understanding of utilization of biomolecules in ORR and materialization of proton exchange membrane fuel cells for clean energy production.

  20. Synthesis of methyl benzoate by methoxycarbonylation of acetophenone with dimethyl carbonate over solid base catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Wu, Dudu; Chang, Wenming; Wen, Xia [State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001 (China); Graduate University of Chinese Academy of Sciences, Beijing, 100039 (China); Xiao, Fukui; Li, Junping; Zhao, Ning; Wei, Wei; Sun, Yuhan [State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001 (China)

    2008-08-15

    A convenient and simple route for synthesis of methyl benzoate from dimethyl carbonate and acetophenone has been exploited for the first time in the presence of solid base catalysts. The results showed that solid base with moderate strength, such as MgO, facilitated the formation of methyl benzoate and the function of basic catalysts could mainly be attributed to the activation of ketone via the abstraction of H{sup {alpha}} by base sites. (author)

  1. Gold Nanoparticles as the Catalyst of Single-Walled Carbon Nanotube Synthesis

    OpenAIRE

    Yoshikazu Homma

    2014-01-01

    Gold nanoparticles have been proven to act as efficient catalysts for chemical reactions, such as oxidation and hydrogen production. In this review we focus on a different aspect of the catalysis of gold nanoparticles; single-walled carbon nanotube (SWCNT) synthesis. This is not a traditional meaning of catalytic reaction, but SWCNTs cannot be synthesized without nanoparticles. Previously, gold was considered as unsuitable metal species as the catalyst of SWCNT synthesis. However, gold nanopa...

  2. Impact of carbon on the surface and activity of silica-carbon supported copper catalysts for reduction of nitrogen oxides

    Science.gov (United States)

    Spassova, I.; Stoeva, N.; Nickolov, R.; Atanasova, G.; Khristova, M.

    2016-04-01

    Composite catalysts, prepared by one or more active components supported on a support are of interest because of the possible interaction between the catalytic components and the support materials. The supports of combined hydrophilic-hydrophobic type may influence how these materials maintain an active phase and as a result a possible cooperation between active components and the support material could occur and affects the catalytic behavior. Silica-carbon nanocomposites were prepared by sol-gel, using different in specific surface areas and porous texture carbon materials. Catalysts were obtained after copper deposition on these composites. The nanocomposites and the catalysts were characterized by nitrogen adsorption, TG, XRD, TEM- HRTEM, H2-TPR, and XPS. The nature of the carbon predetermines the composite's texture. The IEPs of carbon materials and silica is a force of composites formation and determines the respective distribution of the silica and carbon components on the surface of the composites. Copper deposition over the investigated silica-carbon composites leads to formation of active phases in which copper is in different oxidation states. The reduction of NO with CO proceeds by different paths on different catalysts due to the textural differences of the composites, maintaining different surface composition and oxidation states of copper.

  3. Gold Nanoparticles as the Catalyst of Single-Walled Carbon Nanotube Synthesis

    Directory of Open Access Journals (Sweden)

    Yoshikazu Homma

    2014-03-01

    Full Text Available Gold nanoparticles have been proven to act as efficient catalysts for chemical reactions, such as oxidation and hydrogen production. In this review we focus on a different aspect of the catalysis of gold nanoparticles; single-walled carbon nanotube (SWCNT synthesis. This is not a traditional meaning of catalytic reaction, but SWCNTs cannot be synthesized without nanoparticles. Previously, gold was considered as unsuitable metal species as the catalyst of SWCNT synthesis. However, gold nanoparticles with diameters smaller than 5 nm were found to effectively produce SWCNTs. We discuss the catalysis of gold and related metals for SWCNT synthesis in comparison with conventional catalysts, such as iron, cobalt, and nickel.

  4. thesis of high-purity carbon nanotubes over alumina and silica supported bimetallic catalysts

    Directory of Open Access Journals (Sweden)

    Sanja Ratković

    2009-10-01

    Full Text Available Carbon nanotubes (CNTs were synthesized by a catalytic chemical vapor deposition method (CCVD of ethylene over alumina and silica supported bimetallic catalysts based on Fe, Co and Ni. The catalysts were prepared by a precipitation method, calcined at 600 °C and in situ reduced in hydrogen flow at 700 °C. The CNTs growth was carried out by a flow the mixture of C2H4 and nitrogen over the catalyst powder in a horizontal oven. The structure and morphology of as-synthesized CNTs were characterized using SEM. The as-synthesized nanotubes were purified by acid and basic treatments in order to remove impurities such as amorphous carbon, graphite nanoparticles and metal catalysts. XRD and DTA/TG analyses showed that the amounts of by-products in the purified CNTs samples were reduced significantly. According to the observed results, ethylene is an active carbon source for growing high-density CNTs with high yield but more on alumina-supported catalysts than on their silica- supported counterparts. The last might be explained by SMSI formed in the case of alumina-supported catalysts, resulting in higher active phase dispersion.

  5. N-doped carbon nanomaterials are durable catalysts for oxygen reduction reaction in acidic fuel cells.

    Science.gov (United States)

    Shui, Jianglan; Wang, Min; Du, Feng; Dai, Liming

    2015-02-01

    The availability of low-cost, efficient, and durable catalysts for oxygen reduction reaction (ORR) is a prerequisite for commercialization of the fuel cell technology. Along with intensive research efforts of more than half a century in developing nonprecious metal catalysts (NPMCs) to replace the expensive and scarce platinum-based catalysts, a new class of carbon-based, low-cost, metal-free ORR catalysts was demonstrated to show superior ORR performance to commercial platinum catalysts, particularly in alkaline electrolytes. However, their large-scale practical application in more popular acidic polymer electrolyte membrane (PEM) fuel cells remained elusive because they are often found to be less effective in acidic electrolytes, and no attempt has been made for a single PEM cell test. We demonstrated that rationally designed, metal-free, nitrogen-doped carbon nanotubes and their graphene composites exhibited significantly better long-term operational stabilities and comparable gravimetric power densities with respect to the best NPMC in acidic PEM cells. This work represents a major breakthrough in removing the bottlenecks to translate low-cost, metal-free, carbon-based ORR catalysts to commercial reality, and opens avenues for clean energy generation from affordable and durable fuel cells.

  6. N-doped carbon nanomaterials are durable catalysts for oxygen reduction reaction in acidic fuel cells

    Science.gov (United States)

    Shui, Jianglan; Wang, Min; Du, Feng; Dai, Liming

    2015-01-01

    The availability of low-cost, efficient, and durable catalysts for oxygen reduction reaction (ORR) is a prerequisite for commercialization of the fuel cell technology. Along with intensive research efforts of more than half a century in developing nonprecious metal catalysts (NPMCs) to replace the expensive and scarce platinum-based catalysts, a new class of carbon-based, low-cost, metal-free ORR catalysts was demonstrated to show superior ORR performance to commercial platinum catalysts, particularly in alkaline electrolytes. However, their large-scale practical application in more popular acidic polymer electrolyte membrane (PEM) fuel cells remained elusive because they are often found to be less effective in acidic electrolytes, and no attempt has been made for a single PEM cell test. We demonstrated that rationally designed, metal-free, nitrogen-doped carbon nanotubes and their graphene composites exhibited significantly better long-term operational stabilities and comparable gravimetric power densities with respect to the best NPMC in acidic PEM cells. This work represents a major breakthrough in removing the bottlenecks to translate low-cost, metal-free, carbon-based ORR catalysts to commercial reality, and opens avenues for clean energy generation from affordable and durable fuel cells. PMID:26601132

  7. Dehydrogenation of propane in the presence of carbon dioxide over chromium and gallium oxides catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Lapidus, A.L.; Agafonov, Yu.A.; Gaidai, N.A.; Nekrasov, N.V.; Menshova, M.V.; Kunusova, R.M. [Russian Academy of Sciences, Moscow (Russian Federation). N.D. Zelinsky Inst. of Organic Chemistry

    2011-07-01

    Effective chromium and gallium oxides supported catalysts were prepared and tested in longduration experiments for propane dehydrogenation in the presence of CO{sub 2}. The optimal concentrations of active metals were found. It was shown that the activity, selectivity and stability of chromium oxides catalysts were higher than these parameters for gallium ones. Mechanism of propane oxidative dehydrogenation was studied over both catalysts using unstationary and spectroscopic methods. The employment of these methods allowed to establish the differences in process mechanism. It was shown that surface hydroxides took participation in propene formation over Cr-catalysts and hydrides - over Ga-ones. Propane and carbon dioxide participated in the reaction from the adsorbed state over both catalysts but they were differed by the adsorption capacity of the reaction components: CO2 was tied more firmly than C{sub 3}H{sub 6} over both catalysts, CO{sub 2} and C{sub 3}H{sub 6} were tied more strongly with Cr-catalysts than with Ga-ones. It was shown that CO{sub 2} took active participation in reverse watergas shift reaction and in oxidation of catalyst surface over chromium oxides catalysts. The main role of CO{sub 2} in propane dehydrogenation over gallium catalysts consisted in a decrease of coke formation. Step-schemes of propene and cracking products formation were proposed on the basis of literature and obtained data: via the redox mechanism over Cr-catalysts and through a heterolytic dissociation reaction pathway over Ga-ones. (orig.)

  8. CARBON NANOTUBES: PROPERTIES AND APPLICATIONS

    Energy Technology Data Exchange (ETDEWEB)

    Fischer, John, E.

    2009-07-24

    Carbon nanotubes were discovered in 1991 as a minority byproduct of fullerene synthesis. Remarkable progress has been made in the ensuing years, including the discovery of two basic types of nanotubes (single-wall and multi-wall), great strides in synthesis and purification, elucidation of many fundamental physical properties, and important steps towards practical applications. Both the underlying science and technological potential of SWNT can profitably be studied at the scale of individual tubes and on macroscopic assemblies such as fibers. Experiments on single tubes directly reveal many of the predicted quantum confinement and mechanical properties. Semiconductor nanowires have many features in common with nanotubes, and many of the same fundamental and practical issues are in play – quantum confinement and its effect on properties; possible device structures and circuit architectures; thermal management; optimal synthesis, defect morphology and control, etc. In 2000 we began a small effort in this direction, conducted entirely by undergraduates with minimal consumables support from this grant. With DOE-BES approval, this grew into a project in parallel with the carbon nanotube work, in which we studied of inorganic semiconductor nanowire growth, characterization and novel strategies for electronic and electromechanical device fabrication. From the beginnings of research on carbon nanotubes, one of the major applications envisioned was hydrogen storage for fuel-cell powered cars and trucks. Subsequent theoretical models gave mixed results, the most pessimistic indicating that the fundamental H2-SWNT interaction was similar to flat graphite (physisorption) with only modest binding energies implying cryogenic operation at best. New material families with encouraging measured properties have emerged, and materials modeling has gained enormously in predictive power, sophistication, and the ability to treat a realistically representative number of atoms. One of

  9. Advanced Catalysts for the Ambient Temperature Oxidation of Carbon Monoxide and Formaldehyde

    Science.gov (United States)

    Nalette, Tim; Eldridge, Christopher; Yu, Ping; Alpetkin, Gokhan; Graf, John

    2010-01-01

    The primary applications for ambient temperature carbon monoxide (CO) oxidation catalysts include emergency breathing masks and confined volume life support systems, such as those employed on the Shuttle. While Hopcalite is typically used in emergency breathing masks for terrestrial applications, in the 1970s, NASA selected a 2% platinum (Pt) on carbon for use on the Shuttle since it is more active and also more tolerant to water vapor. In the last 10-15 years there have been significant advances in ambient temperature CO oxidation catalysts. Langley Research Center developed a monolithic catalyst for ambient temperature CO oxidation operating under stoichiometric conditions for closed loop carbon dioxide (CO2) laser applications which is also advertised as having the potential to oxidize formaldehyde (HCHO) at ambient temperatures. In the last decade it has been discovered that appropriate sized nano-particles of gold are highly active for CO oxidation, even at sub-ambient temperatures, and as a result there has been a wealth of data reported in the literature relating to ambient/low temperature CO oxidation. In the shorter term missions where CO concentrations are typically controlled via ambient temperature oxidation catalysts, formaldehyde is also a contaminant of concern, and requires specially treated carbons such as Calgon Formasorb as untreated activated carbon has effectively no HCHO capacity. This paper examines the activity of some of the newer ambient temperature CO and formaldehyde (HCHO) oxidation catalysts, and measures the performance of the catalysts relative to the NASA baseline Ambient Temperature Catalytic Oxidizer (ATCO) catalyst at conditions of interest for closed loop trace contaminant control systems.

  10. Removal of free fatty acid in Palm Fatty Acid Distillate using sulfonated carbon catalyst derived from biomass wastefor biodiesel production

    Science.gov (United States)

    Hidayat, Arif; Rochmadi; Wijaya, Karna; Budiman, Arief

    2016-01-01

    In this research, the esterification of PFAD using the sulfonatedcoconut shell biochar catalyst was studied. Carbon solid catalysts were prepared by a sulfonation of carbonized coconut shells. The performances of the catalysts were evaluated in terms of the reaction temperatures, the molar ratios of methanol to PFAD, the catalyst loading and the reaction times. The reusability of the solid acid carbon catalysts was also studied in this work. The results indicated that the FFA conversion was significantly increased with increasing catalyst loading and reaction times. It can be concluded that the optimal conditions were an PFAD to methanol molar ratio of 1:12, the amount of catalyst of 10%w, and reaction temperature of 60oC.At this optimum condition, the conversion to biodieselreached 88%.

  11. Hydrogenation of Glucose Using Ru/Activated Carbon Catalysts: Effects of Modification Methods on Surface Properties of Activated Carbon%葡萄糖加氢用Ru/活性炭催化剂:改性方法对活性炭表面性能的影响

    Institute of Scientific and Technical Information of China (English)

    徐三魁; 李利民; 郭楠楠; 苏运来; 张朋

    2012-01-01

    ).These modifications did not significantly change the surface area and the pore size distribution of the AC.ScCH3OH treatment decreased the density of surface acidic groups,especially carboxylic groups.However,HNO3 oxidation increased the density of surface acidic groups.ICP analysis revealed that the scCH3OH modified sample had a similar adsorptive capacity for ruthenium as the original AC,while the AC oxidized with HNO3 had the highest adsorptive capacity of all samples tested.Ru/AC catalysts were prepared with RuCl3 solution impregnation on the four aforementioned AC supports.The as-prepared catalysts were characterized by TEM,XPS and examined for their effectiveness in D-glucose hydrogenation as well.The modifications drastically affected the properties of the activated carbons and the catalysts loaded on them.The dispersion of ruthenium after impregnation was highly dependent on the density of surface acidic groups.The AC sample treated by scCH3OH,which contained a lower amount of surface acidic complexes,showed the highest dispersion of ruthenium.The XPS results showed that the scCH3OH modification enhanced the interaction between AC and Ru.The Ru/AC-scCH3OH catalyst showed the highest activity for hydrogenation of D-glucose; producing a reaction rate 1.56 times higher than that produced by Ru/AC.

  12. Sustainable production of acetaldehyde from lactic acid over the carbon catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Tang, Congming; Peng, Jiansheng; Li, Xinli; Zhai, Zhanjie; Gao, Hejun; Liao, Yunwen [China West Normal University, Nanchong (China); Bai, Wei; Jiang, Ning [Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu (China)

    2016-01-15

    The synthesis of acetaldehyde from lactic acid over the carbon material catalysts was investigated. The carbon materials were characterized by scanning electron microscopy for morphologic features, by X-ray diffraction for crystal phases, by Fourier transform infrared spectroscopy for functional group structures, by N2 sorption for specific surface area and by ammonia temperature-programed desorption for acidity, respectively. Among the tested carbon catalysts, mesoporous carbon displayed the most excellent catalytic performance. By acidity analysis, the medium acidity is a crucial factor for catalytic performance: more medium acidity favored the formation of acetaldehyde from lactic acid. To verify, we compared the catalytic performance of fresh activated carbon with that of the activated carbon treated by nitric acid. Similarly, the modified activated carbon also displayed better activity due to a drastic increase of medium acidity amount. However, in contrast to fresh carbon nanotube, the treated sample displayed worse activity due to decrease of medium acidity amount. The effect of reaction temperature and time on stream on the catalytic performance was also investigated. Under the optimal reaction conditions, 100% lactic acid conversion and 91.6% acetaldehyde selectivity were achieved over the mesoporous carbon catalyst.

  13. Effects of Temperature and Catalyst Concentration on the Growth of Aligned Carbon Nanotubes

    Institute of Scientific and Technical Information of China (English)

    BAI Xiaodong; LI Dan; WANG Ye; LIANG Ji

    2005-01-01

    The effects of preheating and pyrolysis temperatures and catalyst concentration on the synthesis of aligned carbon nanotubes (CNTs) using ferrocene as the catalyst and xylene as the carbon source in chemical vapor deposition were experimentally studied. The as-grown aligned CNTs were characterized by field emission scanning electron microscopy, transmission electronic microscopy, high-resolution transmission electronic microscopy, and Raman spectroscopy. The growth rate, the diameters, and the degree of crystal structure of the aligned CNTs were all found to depend on the preheating and pyrolysis temperatures and the catalyst concentration. The optimized conditions for the growth of aligned CNTs resulted in a rapid growth rate of 20.4 μm/min, with the CNTs having a good, uniform crystal structure, and clean surfaces with little amorphous carbon. The results also show that higher preheating temperatures and lower ferrocene concentrations favor the growth of single-walled CNTs.

  14. Chemical Properties of Carbon Nanotubes Prepared Using Camphoric Carbon by Thermal-CVD

    International Nuclear Information System (INIS)

    Chemical properties and surface study on the influence of starting carbon materials by using thermal chemical vapor deposition (Thermal-CVD) to produced carbon nanotubes (CNTs) is investigated. The CNTs derived from camphor were synthesized as the precursor material due to low sublimation temperature. The major parameters are also evaluated in order to obtain high-yield and high-quality CNTs. The prepared CNTs are examined using field emission scanning electron microscopy (FESEM) to determine the microstructure of nanocarbons. The FESEM investigation of the CNTs formed on the support catalysts provides evidence that camphor is suitable as a precursor material for nanotubes formation. The chemical properties of the CNTs were conducted using FTIR spectroscopy and PXRD analysis. The high-temperature graphitization process induced by the Thermal-CVD enables the hydrocarbons to act as carbon sources and changes the aromatic species into the layered graphite structure of CNTs.

  15. Chemical Properties of Carbon Nanotubes Prepared Using Camphoric Carbon by Thermal-CVD

    Science.gov (United States)

    Azira, A. A.; Rusop, M.

    2010-03-01

    Chemical properties and surface study on the influence of starting carbon materials by using thermal chemical vapor deposition (Thermal-CVD) to produced carbon nanotubes (CNTs) is investigated. The CNTs derived from camphor were synthesized as the precursor material due to low sublimation temperature. The major parameters are also evaluated in order to obtain high-yield and high-quality CNTs. The prepared CNTs are examined using field emission scanning electron microscopy (FESEM) to determine the microstructure of nanocarbons. The FESEM investigation of the CNTs formed on the support catalysts provides evidence that camphor is suitable as a precursor material for nanotubes formation. The chemical properties of the CNTs were conducted using FTIR spectroscopy and PXRD analysis. The high-temperature graphitization process induced by the Thermal-CVD enables the hydrocarbons to act as carbon sources and changes the aromatic species into the layered graphite structure of CNTs.

  16. Catalytic wet air oxidation of 2-chlorophenol over sewage sludge-derived carbon-based catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Tu, Yuting [Institut de recherches sur la catalyse et l’environnement de Lyon (IRCELYON), CNRS – Université Claude Bernard Lyon 1, 2 Avenue Albert Einstein, 69626 Villeurbanne Cedex (France); School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Xiong, Ya; Tian, Shuanghong [School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Guangzhou 510275 (China); Kong, Lingjun [School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Descorme, Claude, E-mail: claude.descorme@ircelyon.univ-lyon1.fr [Institut de recherches sur la catalyse et l’environnement de Lyon (IRCELYON), CNRS – Université Claude Bernard Lyon 1, 2 Avenue Albert Einstein, 69626 Villeurbanne Cedex (France)

    2014-07-15

    Highlights: • A sewage sludge derived carbon-supported iron oxide catalyst (FeSC) was prepared. • FeSC exhibited high catalytic activity in the wet air oxidation of 2-chlorophenol. • A strong correlation was observed between the 2-CP conversion, the iron leaching and the pH. • Using an acetate buffer, the iron leaching was suppressed while keeping some catalytic activity. • A simplified reaction pathway was proposed for the CWAO of 2-CP over the FeSC catalyst. - Abstract: A sewage sludge derived carbon-supported iron oxide catalyst (FeSC) was prepared and used in the Catalytic Wet Air Oxidation (CWAO) of 2-chlorophenol (2-CP). The catalysts were characterized in terms of elemental composition, surface area, pH{sub PZC}, XRD and SEM. The performances of the FeSC catalyst in the CWAO of 2-CP was assessed in a batch reactor operated at 120 °C under 0.9 MPa oxygen partial pressure. Complete decomposition of 2-CP was achieved within 5 h and 90% Total Organic Carbon (TOC) was removed after 24 h of reaction. Quite a straight correlation was observed between the 2-CP conversion, the amount of iron leached in solution and the pH of the reaction mixture at a given reaction time, indicating a strong predominance of the homogeneous catalysis contribution. The iron leaching could be efficiently prevented when the pH of the solution was maintained at values higher than 4.5, while the catalytic activity was only slightly reduced. Upon four successive batch CWAO experiments, using the same FeSC catalyst recovered by filtration after pH adjustment, only a very minor catalyst deactivation was observed. Finally, based on all the identified intermediates, a simplified reaction pathway was proposed for the CWAO of 2-CP over the FeSC catalyst.

  17. Study on Carbon Nanotubes Prepared from Catalytic Decomposition of CH4 over Lanthanum Containing Ni-Base Catalysts

    Institute of Scientific and Technical Information of China (English)

    Wang Minwei; Li Fengyi

    2004-01-01

    A series of lanthanum containing Ni-base catalysts were prepared by citric acid complex method.Carbon nanotubes (CNT) were synthesized bY catalytic decomposing CH4 over these catalysts and characterized by XRD, TEM and TGA.It is found that the addition of lanthanum can not increase the yield of carbon nanotube, but can make the diameter of carbon nanotube thinner and even.The more the lanthanum addsr, the thinner the diameter of CNTs becomes.With the CNTs prepared on Ni-Mg catalyst, the CNTs prepared on Ni-La-Mg catalyst has better crystallinity and thermal stability.

  18. Efficient Nd Promoted Rh Catalysts for Vapor Phase Methanol Carbonylation

    Institute of Scientific and Technical Information of China (English)

    Shu Feng ZHANG; Qing Li QIAN; Ping Lai PAN; Yi CHEN; Guo Qing YUAN

    2005-01-01

    A Nd promoted-Rh catalysts supported on polymer-derived carbon beads for vapor-phase methanol carbonylation was developed. Rh-Nd bimetallic catalysts obviously have higher activity than that of supported Rh catalyst under similar reaction condition. The difference between the activity of above two catalyst systems is clearly caused by the intrinsic properties generated by the introduction of Nd.

  19. Synthesis of multi-walled carbon nanotubes using CoMnMgO catalysts through catalytic chemical vapor deposition

    Science.gov (United States)

    Yang, Wen; Feng, Yan-Yan; Jiang, Cheng-Fa; Chu, Wei

    2014-12-01

    The CoMgO and CoMnMgO catalysts are prepared by a co-precipitation method and used as the catalysts for the synthesis of carbon nanotubes (CNTs) through the catalytic chemical vapor deposition (CCVD). The effects of Mn addition on the carbon yield and structure are investigated. The catalysts are characterized by temperature programmed reduction (TPR) and X-ray diffraction (XRD) techniques, and the synthesized carbon materials are characterized by transmission electron microscopy (TEM) and thermo gravimetric analysis (TG). TEM measurement indicates that the catalyst CoMgO enclosed completely in the produced graphite layer results in the deactivation of the catalyst. TG results suggest that the CoMnMgO catalyst has a higher selectivity for CNTs than CoMgO. Meanwhile, different diameters of CNTs are synthesized by CoMnMgO catalysts with various amounts of Co content, and the results show that the addition of Mn avoids forming the enclosed catalyst, prevents the formation of amorphous carbon, subsequently promotes the growth of CNTs, and the catalyst with decreased Co content is favorable for the synthesis of CNTs with a narrow diameter distribution. The CoMnMgO catalyst with 40% Co content has superior catalytic activity for the growth of carbon nanotubes.

  20. Synthesis of Nitrogen-Doped Carbon Nanocoils with Adjustable Morphology using Ni–Fe Layered Double Hydroxides as Catalyst Precursors

    OpenAIRE

    Tomohiro Iwasaki; Masashi Tomisawa; Takuma Yoshimura; Hideya Nakamura; Masao Ohyama; Katsuya Asao; Satoru Watano

    2015-01-01

    Nitrogen-doped carbon nanocoils (CNCs) with adjusted morphologies were synthesized in a one-step catalytic chemical vapour deposition (CVD) process using acetoni‐ trile as the carbon and nitrogen source. The nickel iron oxide/nickel oxide nanocomposites, which were derived from nickel–iron layered double hydroxide (LDH) precur‐ sors, were employed as catalysts for the synthesis of CNCs. In this method, precursor-to-catalyst transformation, catalyst activation, formation of CNCs, and nitrogen ...

  1. A rational design approach to nanostructured catalysts for the oxidation of carbon monoxide

    Science.gov (United States)

    Karwacki, Christopher

    The extraordinary energetic properties of subnanometer (model for the nanosciences, where molecular species are synthesized, scaled, and engineered into functional materials. Gold nanoparticles as isolated structures are not useful as real catalysts and must co-exist with supports that provide enhanced stability and activity. Support oxides such as TiO2, Fe2O 3, CeO2, SiO2, Al2O3, ZrO 2, and graphitic (active) carbons have been shown to increase the active nature of AuNP and have been the subject of several thousand publications in the past decade. Zirconia compared to titania as a support for Au NP catalysis has been studied with limited success. In fact, the majority of observations show that zirconia is one of the lowest performing metal oxide supports involving Au NP oxidation catalysis. The likely reason for these observations is a lack of understanding of the relationship between structure and surface functionality as it pertains to ambient temperature oxidation catalysis (ATOC). Furthermore, virtually all substrate and catalyst preparations in earlier work were performed at high temperatures, typically 400--900°C, thus forming progressively monomorphic structures containing larger crystals with reduced surface functionality and porosity. In this research, I established the hypothesis based on a structural model that surface functional hydroxides are important to sustained hydrolytic reactions, such as those involving Au NP for the oxidation of CO to CO 2. Theoretical calculations by Ignatchenko, Vittadini, et al. show that zirconia readily dissociates adsorbed water on the most active and stable crystal structures (111) compared to other metal oxides, such as the common anatase (101) form of titania. Also, the support must provide a source of activated oxygen as a means to oxidize intermediate carbonates with CO 2 formation. The role of the support is to provide lattice oxygen in an activated state (O2-) for oxidation of adsorbed CO the Au NP

  2. Carbon/H-ZSM-5 composites as supports for bi-functional Fischer-Tropsch synthesis catalysts

    NARCIS (Netherlands)

    Valero-Romero, M.J.; Sartipi, S.; Sun, X.; Rodríguez-Mirasol, J.; Cordero, T.; Kapteijn, F.; Gascon, J.

    2016-01-01

    Mesoporous H-ZSM-5–carbon composites, prepared via tetrapropylammonium hydroxide (TPAOH) post treatment of H-ZSM-5 followed by deposition of pyrolytic carbon, have been used as the support for the preparation of Co-based Fischer–Tropsch catalysts. The resulting catalysts display an improved performa

  3. Enhanced Activity and Selectivity of Carbon Nanofiber Supported Pd Catalysts for Nitrite Reduction

    KAUST Repository

    Shuai, Danmeng

    2012-03-06

    Pd-based catalyst treatment represents an emerging technology that shows promise to remove nitrate and nitrite from drinking water. In this work we use vapor-grown carbon nanofiber (CNF) supports in order to explore the effects of Pd nanoparticle size and interior versus exterior loading on nitrite reduction activity and selectivity (i.e., dinitrogen over ammonia production). Results show that nitrite reduction activity increases by 3.1-fold and selectivity decreases by 8.0-fold, with decreasing Pd nanoparticle size from 1.4 to 9.6 nm. Both activity and selectivity are not significantly influenced by Pd interior versus exterior CNF loading. Consequently, turnover frequencies (TOFs) among all CNF catalysts are similar, suggesting nitrite reduction is not sensitive to Pd location on CNFs nor Pd structure. CNF-based catalysts compare favorably to conventional Pd catalysts (i.e., Pd on activated carbon or alumina) with respect to nitrite reduction activity and selectivity, and they maintain activity over multiple reduction cycles. Hence, our results suggest new insights that an optimum Pd nanoparticle size on CNFs balances faster kinetics with lower ammonia production, that catalysts can be tailored at the nanoscale to improve catalytic performance for nitrite, and that CNFs hold promise as highly effective catalyst supports in drinking water treatment. © 2012 American Chemical Society.

  4. Application of Ce{sub x}Zr{sub 1-x}O{sub 2} catalysts for the synthesis of diethyl carbonate from ethanol and carbon dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Prymak, I.; Kalevaru, V.N.; Kollmorgen, P.; Wohlrab, S. [Leibniz-Institut fuer Katalyse e.V. an der Universitaet Rostock (Germany); Martin, A.

    2013-11-01

    The direct synthesis of diethyl carbonate (DEC) from ethanol and CO{sub 2} is indeed an attractive approach from both academic and commercial points of view. In the present study, we report on the synthesis, characterization and catalytic evaluation of Ce-Zr-O solids with varying Ce/Zr ratios. The catalysts were prepared by citrate complexation method, and characterized by various techniques such as N{sub 2} adsorption (BET-SA), XRD, H{sub 2}-TPR, NH{sub 3}-TPD etc. The catalytic performance of these catalysts was evaluated towards the synthesis of DEC from ethanol and CO{sub 2} under suitable reaction conditions. According to thermodynamic data, the reaction is favorable at low reaction temperatures and high reaction pressures. Thus, the catalytic experiments were carried out in a continuous mode using a plug-flow reactor that was operated up to 200 bar and ca. 200 C. The effect of the reaction temperature (30-180 C) and pressure (80-180 bar) on the yield of DEC was investigated. Among various catalysts tested, Ce-Zr-O catalyst with 80 mol% Ce content has exhibited a relatively better performance compared to all other Ce-Zr-O catalysts. DEC yield increased with increasing reaction temperature up to 140 C. The highest yield of DEC obtained from the best case was 0.7 % at 140 C and at 140 bars. Further increase in temperature to 180 C caused a decrease in the DEC formation due to thermodynamic reasons as mentioned above. The ceria proportion has shown a considerable influence on the BET surface areas and thereby catalytic activity as well. The results revealed that the redox properties as well as acidity characteristics of the solids are strongly influenced by the content of Ce in the catalysts, which in turn showed a clear impact on the catalytic performance. (orig.)

  5. Characterization of platinum catalyst supported on carbon nanoballs prepared by solution plasma processing

    International Nuclear Information System (INIS)

    In order to improve the energy-conversion efficiency in fuel cells, the authors loaded Pt nanoparticles on carbon nanoballs (CNBs) by using solution plasma processing (SPP) involving CNB and Pt ion with a protection group. In this study, we employed poly(vinylpyrrolidone) (PVP) or sodium dodecyl sulfate (SDS) to prepare Pt nanoparticles supported on CNB (Pt/CNB) by the SPP, and the electrochemical properties as a catalyst was evaluated by cyclic voltammetry. The carbon nanoballs were prepared by thermal decomposition process of ethylene and hydrogen gases. Color of the solution changed from yellow to dark brown as synthesis time. This change indicates the improvement of dispersibility of CNB. Moreover, transmission electron microscopy images and elemental mapping images showed the Pt nanoparticles supported on CNB. A catalytic activity of the Pt/CNB in use of SDS was shown to be higher than the Pt/CNB prepared with PVP system. The SDS-containing Pt/CNB also showed the higher activity than that obtained by the conventional method.

  6. Flexible, highly graphitized carbon aerogels based on bacterial cellulose/lignin: Catalyst-free synthesis and its application in energy storage devices

    KAUST Repository

    Xu, Xuezhu

    2015-04-15

    Currently, most carbon aerogels are based on carbon nanotubes (CNTs) or graphene, which are produced through a catalyst-assisted chemical vapor deposition method. Biomass based organic aerogels and carbon aerogels, featuring low cost, high scalability, and small environmental footprint, represent an important new research direction in (carbon) aerogel development. Cellulose and lignin are the two most abundant natural polymers in the world, and the aerogels based on them are very promising. Classic silicon aerogels and available organic resorcinol-formaldehyde (RF) or lignin-resorcinol-formaldehyde (LRF) aerogels are brittle and fragile; toughening of the aerogels is highly desired to expand their applications. This study reports the first attempt to toughen the intrinsically brittle LRF aerogel and carbon aerogel using bacterial cellulose. The facile process is catalyst-free and cost-effective. The toughened carbon aerogels, consisting of blackberry-like, core-shell structured, and highly graphitized carbon nanofibers, are able to undergo at least 20% reversible compressive deformation. Due to their unique nanostructure and large mesopore population, the carbon materials exhibit an areal capacitance higher than most of the reported values in the literature. This property makes them suitable candidates for flexible solid-state energy storage devices. Besides energy storage, the conductive interconnected nanoporous structure can also find applications in oil/water separation, catalyst supports, sensors, and so forth. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. A novel method for fabrication of Fe catalyst used for the synthesis of carbon nanotubes

    Indian Academy of Sciences (India)

    E Z Karimi; J Vahdati-Khaki; S M Zebarjad; I A Bataev; A G Bannov

    2014-08-01

    Carbon nanotubes (CNTs) have been grown by decomposition of propane over a nanocamposite catalyst by chemical vapour deposition (CVD). The catalyst was prepared from an aluminum/iron oxide/graphite mixture milled in a high-energy ball-milling equipment. Scanning and transmission electron microscopies, Raman spectroscopy and X-ray diffraction measurements have been carried out in order to investigate the catalyst and synthesized CNTs. The results show that iron nanoparticles are produced in an alumina and ball-milled graphite matrix. This produced nanocomposite is used as a catalyst to synthesize CNTs via CVD successfully. The yield of CNTs formation was greatly influenced by the milling time and deposition temperature.

  8. Monodispersed Hollow SO3H-Functionalized Carbon/Silica as Efficient Solid Acid Catalyst for Esterification of Oleic Acid.

    Science.gov (United States)

    Wang, Yang; Wang, Ding; Tan, Minghui; Jiang, Bo; Zheng, Jingtang; Tsubaki, Noritatsu; Wu, Mingbo

    2015-12-01

    SO3H-functionalized monodispersed hollow carbon/silica spheres (HS/C-SO3H) with primary mesopores were prepared with polystyrene as a template and p-toluenesulfonic acid (TsOH) as a carbon precursor and -SO3H source simultaneously. The physical and chemical properties of HS/C-SO3H were characterized by N2 adsorption, TEM, SEM, XPS, XRD, Raman spectrum, NH3-TPD, element analysis and acid-base titration techniques. As a solid acid catalyst, HS/C-SO3H shows excellent performance in the esterification of oleic acid with methanol, which is a crucial reaction in biodiesel production. The well-defined hollow architecture and enhanced active sites accessibility of HS/C-SO3H guarantee the highest catalytic performance compared with the catalysts prepared by activation of TsOH deposited on the ordered mesoporous silicas SBA-15 and MCM-41. At the optimized conditions, high conversion (96.9%) was achieved and no distinct activity drop was observed after 5 recycles. This synthesis strategy will provide a highly effective solid acid catalyst for green chemical processes. PMID:26588826

  9. Metal–organic framework-based catalysts: Chemical fixation of CO2 with epoxides leading to cyclic organic carbonates

    Directory of Open Access Journals (Sweden)

    M. Hassan eBeyzavi

    2015-01-01

    Full Text Available As a C1 feedstock, CO2 has the potential to be uniquely highly economical in both a chemical and a financial sense. In particular, the highly atom-economical acid-catalyzed cycloaddition of CO2 to epoxides to yield cyclic organic carbonates (OCs, a functionality having many important industrial applications, is an attractive reaction for the utilization of CO2 as a chemical feedstock. Metal–organic frameworks (MOFs are promising candidates in catalysis as they are a class of crystalline, porous and functional materials with remarkable properties including great surface area, high stability, open channels and permanent porosity. MOFs structure tunability and their affinity for CO2, makes them great catalysts for the formation of OCs using CO2 and epoxides. In this review, we examine MOF-based catalytic materials for the cycloaddition of carbon dioxide to epoxides. Catalysts are grouped based on the location of catalytic sites, i.e., at the struts, nodes, defect sites, or some combination thereof. Additionally, important features of each catalyst system are critically discussed.

  10. Physico-Chemical and Structural Properties of DeNOx and SO2 Oxidation Catalysts

    DEFF Research Database (Denmark)

    Masters, Stephen Grenville; Oehlers, Cord; Nielsen, Kurt;

    1996-01-01

    Commercial catalysts for NOx removal and SO2 oxidation and their model systems have been investigated by spectroscopic, thermal, electrochemical and X-ray methods. Structural information on the vanadium complexes and compounds as well as physico-chemical properties for catalyst model systems have...... been obtained. The results are discussed in relation to proposed reaction mechanisms....

  11. Electro-Deposition Pt Catalysts Supported on Carbon-Nanotubes for Methanol Oxidation

    Institute of Scientific and Technical Information of China (English)

    Hailin Song; Peixia Yang; Xiaoyu Wen; Maozhong An; Jinqiu Zhang

    2015-01-01

    In order to study the properties of supporting Pt catalysts for methanol oxidation, carbon⁃nanotubes are used by electrochemical deposition method. Different deposition turns, different cyclic voltammetry scanning speeds and processing time with ascorbic acid are investigated in this paper. The micrographs of Pt/CNTs catalysts are characterized by scanning electron microscopy, the electro⁃catalytic properties of Pt/CNTs catalysts for methanol oxidation are investigated by cycle voltammetry and chronoamperometry. The results show that the size of platinum will be greater with the faster scanning speed. After dissolution in ascorbic acid, Pt nano⁃particles disperse uniformly. The obtained Pt/CNTs catalysts show a high electro⁃catalytic activity and stability.

  12. Production of Carbon Nanofibers Using a CVD Method with Lithium Fluoride as a Supported Cobalt Catalyst

    Directory of Open Access Journals (Sweden)

    S. A. Manafi

    2008-01-01

    Full Text Available Carbon nanofibers (CNFs have been synthesized in high yield (>70% by catalytic chemical vapor deposition (CCVD on Co/LiF catalyst using acetylene as carbon source. A novel catalyst support (LiF is reported for the first time as an alternative for large-scale production of carbon nanofibers while purification process of nanofibers is easier. In our experiment, the sealed furnace was heated at 700∘C for 0.5 hour (the heating rate was 10∘C/min and then cooled to room temperature in the furnace naturally. Catalytic chemical vapor deposition is of interest for fundamental understanding and improvement of commercial synthesis of carbon nanofibers (CNFs. The obtained sample was sequentially washed with ethanol, dilutes acid, and distilled water to remove residual impurities, amorphous carbon materials, and remaining of catalyst, and then dried at 110∘C for 24 hours. The combined physical characterization through several techniques, such as high-resolution transmission electron microscope (TEM, scanning electron microscope (SEM, thermogarvimetric analysis (TGA, and zeta-sizer and Raman spectroscopy, allows determining the geometric characteristic and the microstructure of individual carbon nanofibers. Catalytic chemical vapor deposition is of interest for fundamental understanding and improvement of commercial synthesis of carbon nanofibers (CNFs. As a matter of fact, the method of CCVD guarantees the production of CNFs for different applications.

  13. The Thermodynamic Properties and Homogeneous Catalysts for the Synthesis of Diphenyl Carbonate by Transesterification of Dimethyl Carbonate with Phenol%碳酸二甲酯与苯酚酯交换合成碳酸二苯酯的热力学性质及均相催化剂

    Institute of Scientific and Technical Information of China (English)

    梅付名; 李光兴

    2003-01-01

    The Gibbs free energy of formation and entropy of liquid dimethyl carbonate(DMC) at 298.15K and 101.325kPa were estimated to be -472.3 kJ*mol-1 and 245.2 J*mol-1*K-1 respectively. The thermodynamic properties (ΔrH0m,ΔrS0m,ΔrG0m and equilibrium constant) of the reactions for the production of diphenyl carbonate(DPC) and anisole between DMC and phenol from 298K to 523K were calculated. These values indicated that the reaction of transesterification of DMC with phenol to DPC was endothermic and thermodynamically unfavorable. n-Bu2SnO, Ti(OC4H9)4, AlCl3 and ZnCl2 were tested to catalyze the synthesis of DPC by transesterification of DMC with phenol. n-Bu2SnO had the highest catalytic activity among them. The optimum temperature was 453K for the synthesis of DPC. When the molar ratio of phenol to dimethyl carbonate was 4∶1, the yield and selectivity of DPC were 43.0% and 88.7% respectively using n-Bu2SnO as a catalyst.%在298.15K,101.325kPa条件下,液态碳酸二甲酯(DMC)的标准Gibbs自由能和熵分别估算为-472.3kJ*mol-1和245.2J*mol-1*K-1.在298K~523K计算了由DMC和苯酚生成碳酸二苯酯(DPC)和苯甲醚反应的热力学性质(ΔrH0m,ΔrS0m,ΔrG0m和平衡常数).计算出的热力学性质表明,DMC和苯酚酯交换合成DPC反应是吸热的,并且在热力学上是不利的.研究了n-Bu2SnO, Ti(OC4H9)4, AlCl3和ZnCl2四种酯交换法合成DPC反应的催化剂,其中n-Bu2SnO具有最高的催化活性.热力学计算和实验结果均表明,合成DPC反应的最佳温度为453K.当以n-Bu2SnO为催化剂,n(苯酚)∶n(DMC)=4∶1时,DPC的产率和选择性分别为43.0%和88.7%.

  14. Carbon Materials as Catalysts for Decomposition and CO2 Reforming of Methane: A Review%用于甲烷分解和甲烷二氧化炭重整的碳材料催化剂研究进展

    Institute of Scientific and Technical Information of China (English)

    Beatriz FIDALGO; J.(A)ngel MEN(E)NDEZ

    2011-01-01

    The decomposition and CO2 reforming of methane, respectively, are promising altematives to industrial steam methane reforming. In recent years, research has been focused on the development of catalysts that can operate without getting deactivated by carbon deposition, where, in particular, carbon catalysts have shown positive results. In this work,the role of carbon materials in heterogeneous catalysis is assessed and publications on methane decomposition and CO2 reforming of methane over carbon materials are reviewed. The influence of textural properties (BET surface area and micropore volume, etc.) and oxygen surface groups on the catalytic activity of carbon materials are discussed. In addition. this review examines how activated carbon and carbon black catalysts. which are the most commonly used carbon catalysts, are deactivated. Characteristics of the carbon deposits from methane are discussed and the influence of the reactivity to CO2 of fresh carbon and carbonaceous deposits for high and steady conversion during CO2 reforming of CH4 are also considered.

  15. New Catalyst Reduces Wasted Carbon in Biofuel Process, Lowers Cost

    Energy Technology Data Exchange (ETDEWEB)

    2016-02-01

    Researchers at NREL recently developed a catalyst formulation that incorporates more hydrogen into the DME-to-high-octane gasoline process, resulting in a higher yield to gasoline-range products. Further, the researchers developed a secondary process that efficiently couples a portion of the gasoline-range product to yield jet/diesel fuels. The modified catalyst doubles the conversion rate of DME, which can be produced from biomass, to the high-octane gasoline product and significantly decreases the formation of wasted byproducts. For the distillate-range product, 80% of the mixture is in line with ASTM standards for use as a jet fuel blendstock. The increased productivity of high-octane gasoline and the development of a value-added distillate blendstock process further improve the economic viability toward commercially implementing this renewable fuels process.

  16. CO{sub x}-free hydrogen and carbon nanofibers production by methane decomposition over nickel-alumina catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Bayat, Nima; Rezaei, Mehran; Meshkani, Fereshteh [Faculty of Engineering, University of Kashan, Kashan (Iran, Islamic Republic of)

    2016-02-15

    Nickel catalysts supported on mesoporous nanocrystalline gamma alumina with various nickel loadings were prepared and employed for thermocatalytic decomposition of methane into CO{sub x}-free hydrogen and carbon nanofibers. The prepared catalysts with different nickel contents exhibited mesoporous structure with high surface area in the range of 121.3 to 66.2m{sup 2}g{sup -1}. Increasing in nickel content decreased the pore volume and increased the crystallite size. The catalytic results revealed that the nickel content and operating temperature both play important roles on the catalytic performance of the prepared catalysts. The results showed that increasing in reaction temperature increased the initial conversion of catalysts and significantly decreased the catalyst lifetime. Scanning electron microscopy (SEM) analysis of the spent catalysts evaluated at different temperatures revealed the formation of intertwined carbon filaments. The results showed that increasing in reaction temperature decreased the diameters of nanofibers and increased the formation of encapsulating carbon.

  17. Catalytic conversion of xylose and corn stalk into furfural over carbon solid acid catalyst in γ-valerolactone.

    Science.gov (United States)

    Zhang, Tingwei; Li, Wenzhi; Xu, Zhiping; Liu, Qiyu; Ma, Qiaozhi; Jameel, Hasan; Chang, Hou-min; Ma, Longlong

    2016-06-01

    A novel carbon solid acid catalyst was synthesized by the sulfonation of carbonaceous material which was prepared by carbonization of sucrose using 4-BDS as a sulfonating agent. TEM, N2 adsorption-desorption, elemental analysis, XPS and FT-IR were used to characterize the catalyst. Then, the catalyst was applied for the conversion of xylose and corn stalk into furfural in GVL. The influence of the reaction time, temperature and dosage of catalyst on xylose dehydration were also investigated. The Brønsted acid catalyst exhibited high activity in the dehydration of xylose, with a high furfural yield of 78.5% at 170°C in 30min. What's more, a 60.6% furfural yield from corn stalk was achieved in 100min at 200°C. The recyclability of the sulfonated carbon catalyst was perfect, and it could be reused for 5times without the loss of furfural yields.

  18. Application of mesoporous catalysts over palm-oil biodiesel for adjusting fuel properties

    International Nuclear Information System (INIS)

    Highlights: ► The catalysts MCM-41 and SiO2/Fe3O4 were used to reduce the low-temperature fluidity of biodiesel. ► The catalyst SiO2/Fe3O4 was found to be more effective than MCM-41 for dehydrogenation and cracking reaction. ► Biodiesel had a lower water formation rate when the catalysts were used in the reaction. ► Biodiesel catalyzed by SiO2/Fe3O4 at 600 °C produced the lowest CFPP and the highest iodine value. - Abstract: Biodiesel has superior fuel characteristics, including a higher flash point, better lubricity, and higher oxygen content, and is thus considered a promising alternative clean fuel to petroleum diesel. The cold filter plugging point (CFPP) is the most significant indicator of the low-temperature fluidity of biodiesel. The CFPP of biodiesel is generally higher than that of petroleum diesel primarily due to the longer carbon-chain structures of the fatty acids in the former. Raw materials such as palm oil and waste cooking oil are widely used as the feedstock to produce biodiesel because of their low cost, good availability, and stable lipid provision. However, they generally have a poor low-temperature fluidity, which limits their application in colder climates. In this experimental study, the catalytic dehydrogenation and cracking reaction technique was used to reduce the CFPP of palm-oil biodiesel with an initial CFPP of as high as 14 °C. The catalytic variables of the type of mesoporous catalyst and operating temperature are considered in this study. The resultant fuel properties of palm-oil biodiesel catalyzed by MCM-41 and SiO2/Fe3O4 were compared with biodiesel thermally cracked without a catalyst. The operating temperature of the catalyzed dehydrogenation and cracking reaction was controlled in the range between 400 and 600 °C. The CFPP decrease reached a maximum of 12 °C when the biodiesel was catalyzed by SiO2/Fe3O4 at 600 °C. The maximum water content was produced when the biodiesel sample was thermally cracked with no

  19. Doped carbon nanostructures as metal-free catalysts for oxidative dehydrogenation of light alkanes

    OpenAIRE

    Jenssen, Kaia Andersson

    2014-01-01

    Catalytic reactions are often carried out on various supported metals, these usually being noble metals or metal oxides. Even though metal based catalysts plays a major role in today s industrial processes, they still have several disadvantages, including high cost, proneness to gas poisoning, as well as disadvantageous effect on the environment. Recently, certain carbon nanomaterials have been in the spotlight of several research groups, as carbon has the advantages of wide availability, env...

  20. Carboxylic Group Embedded Carbon Balls as a New Supported Catalyst for Hydrogen Economic Reactions.

    Science.gov (United States)

    Bordoloi, Ankur

    2016-03-01

    Carboxylic group functionalized carbon balls have been successfully synthesized by using a facile synthesis method and well characterized with different characterization techniques such as XPS, MAS NMR, SEM, ICP and N2 physi-sorption analysis. The synthesized material has been effectively utilized as novel support to immobilized ruthenium catalyst for hydrogen economic reactions. PMID:27455763

  1. Catalytic oxidation of pulping effluent by activated carbon-supported heterogeneous catalysts.

    Science.gov (United States)

    Yadav, Bholu Ram; Garg, Anurag

    2016-01-01

    The present study deals with the non-catalytic and catalytic wet oxidation (CWO) for the removal of persistent organic compounds from the pulping effluent. Two activated carbon-supported heterogeneous catalysts (Cu/Ce/AC and Cu/Mn/AC) were used for CWO after characterization by the following techniques: temperature-programmed reduction, Fourier transform infrared spectroscopy and thermo-gravimetric analysis. The oxidation reaction was performed in a batch high-pressure reactor (capacity = 0.7  L) at moderate oxidation conditions (temperature = 190°C and oxygen pressure = 0.9 MPa). With Cu/Ce/AC catalyst, the maximum chemical oxygen demand (COD), total organic carbon (TOC) and lignin removals of 79%, 77% and 88% were achieved compared to only 50% removal during the non-catalytic process. The 5-day biochemical oxygen demand (BOD5) to COD ratio (a measure for biodegradability) of the pulping effluent was improved to 0.52 from an initial value of 0.16. The mass balance calculations for solid recovered after CWO reaction showed 8% and 10% deduction in catalyst mass primarily attributed to the loss of carbon and metal leaching. After the CWO process, carbon deposition was also observed on the recovered catalyst which was responsible for around 3-4% TOC reduction. PMID:26508075

  2. Selective formation of diamond-like carbon coating by surface catalyst patterning

    DEFF Research Database (Denmark)

    Palnichenko, A.V.; Mátéfi-Tempfli, M.; Mátéfi-Tempfli, Stefan;

    2004-01-01

    The selective formation of diamond-like carbon coating by surface catalyst patterning was studied. DLC films was deposited using plasma enhanced chemical vapor deposition, filtered vacuum arc deposition, laser ablation, magnetron sputtering and ion-beam lithography methods. The DLC coatings were...

  3. Carbon Supported Polyaniline as Anode Catalyst: Pathway to Platinum-Free Fuel Cells

    CERN Document Server

    Zabrodskii, A G; Malyshkin, V G; Sapurina, I Y

    2006-01-01

    The effectiveness of carbon supported polyaniline as anode catalyst in a fuel cell (FC) with direct formic acid electrooxidation is experimentally demonstrated. A prototype FC with such a platinum-free composite anode exhibited a maximum room-temperature specific power of about 5 mW/cm2

  4. Carboxylic Group Embedded Carbon Balls as a New Supported Catalyst for Hydrogen Economic Reactions.

    Science.gov (United States)

    Bordoloi, Ankur

    2016-03-01

    Carboxylic group functionalized carbon balls have been successfully synthesized by using a facile synthesis method and well characterized with different characterization techniques such as XPS, MAS NMR, SEM, ICP and N2 physi-sorption analysis. The synthesized material has been effectively utilized as novel support to immobilized ruthenium catalyst for hydrogen economic reactions.

  5. Phosphorylated mesoporous carbon as effective catalyst for the selective fructose dehydration to HMF

    Energy Technology Data Exchange (ETDEWEB)

    Villa, Alberto [Universita di Milano, Italy; Schiavoni, Marco [University of Milan and INFN, Milano, Italy; Fulvio, Pasquale F [ORNL; Mahurin, Shannon Mark [ORNL; Dai, Sheng [ORNL; Mayes, Richard T [ORNL; Veith, Gabriel M [ORNL; Prati, Laura [Universita di Milano, Italy

    2013-01-01

    Phosphorylated mesoporous carbons (PMCs) have been synthesized using an already reported one pot methodology. These materials have been applied as acidic catalysts in the dehydration of fructose to hydroxymethylfurfural (HMF). PMCs showed better selectivity to HMF compared to sulfonated carbon catalyst (SC) despite lower activity. The concentration of P-O groups correlates to the activity/selectivity of the catalysts; the higher the P-O concentration the higher the activity. However, the higher the P-O content the lower the selectivity to HMF. Indeed a lower concentration of the P-O groups (and even the acidic groups) minimized the degradation of HMF to levulinic acid and the formation of by-products, such as humines. Stability tests showed that these systems deactivate due to the formation of humines, water insoluble by-products derived from the dehydration of fructose, blocking the active site of the catalyst. Increasing the amount of P-O groups, higher amount of humines are formed; therefore carbons containing lower amount of phosphorylated groups, such as P/N-0.25, are less prone to deactivation. Keywords: Phosphorylated mesoporous carbons; fructose dehydration; HMF

  6. Oxygen reduction on carbon supported platinum catalysts in high temperature polymer electrolytes

    DEFF Research Database (Denmark)

    Qingfeng, Li; Hjuler, Hans Aage; Bjerrum, Niels

    2000-01-01

    Oxygen reduction on carbon supported platinum catalysts has been investigated in H3PO4, H3PO4-doped Nafion and polybenzimidazole (PBI) polymer electrolytes in a temperature range up to 190 degrees C. Compared with pure H3PO4, the combination of H3PO4 and polymer electrolytes can significantly imp...

  7. Oxygen reduction on carbon supported platinum catalysts in high temperature polymer electrolytes

    DEFF Research Database (Denmark)

    Qingfeng, Li; Bergqvist, R. S.; Hjuler, H. A.;

    1999-01-01

    Oxygen reduction on carbon supported platinum catalysts has been investigated in H3PO4, H3PO4-doped Nafion and PBI polymer electrolytes in a temperature range from 80 to 190°C. Compared with pure H3PO4, using the H3PO4 doped Nafion and PBI polymer electrolytes can significantly improve the oxygen...

  8. Electrocatalytic activity of atomic layer deposited Pt–Ru catalysts onto N-doped carbon nanotubes

    DEFF Research Database (Denmark)

    Johansson, Anne-Charlotte Elisabeth Birgitta; Larsen, Jackie Vincent; Verheijen, Marcel A.;

    2014-01-01

    Pt–Ru catalysts of various compositions, between 0 and 100at.% of Ru, were deposited onto N-doped multi-walled carbon nanotubes (N-CNTs) by atomic layer deposition (ALD) at 250°C. The Pt and Ru precursors were trimethyl(methylcyclopentadienyl)platinum (MeCpPtMe3) and bis...

  9. Effect of hydrogen plasma irradiation of catalyst films on growth of carbon nanotubes filled with iron nanowires

    Energy Technology Data Exchange (ETDEWEB)

    Sato, Hideki, E-mail: sato@elec.mie-u.ac.jp; Kubonaka, Nobuo; Nagata, Atsushi; Fujiwara, Yuji [Graduate School of Engineering, Mie University, 1577 Kurima-machiya-cho, Tsu 514-8507 (Japan)

    2014-03-15

    Carbon nanotubes filled with iron (Fe-filled CNTs) show shape anisotropy on account of the high aspect ratio of magnetic nanowires, and are promising candidates for various applications, such as magnetic recording media, probes for scanning force microscopy, and medical treatment for cancer. The ability to appropriately control the magnetic properties of CNTs for those applications is desirable. In this study, the authors investigated magnetic properties of Fe-filled CNTs synthesized by thermal chemical vapor deposition for the purpose of tuning their coercivity. Here, the authors implemented hydrogen plasma irradiation of catalyst film that was previously deposited on a substrate as a catalyst layer. This treatment activates the catalyst film and thus enhances the growth of the Fe-filled CNTs. It was confirmed that the H{sub 2} plasma irradiation enhances the growth of the CNTs in terms of increasing their length and diameter compared to CNTs without irradiation. On the other hand, the coercivity of Fe-filled CNTs dropped to approximately half of those without H{sub 2} plasma irradiation. This is probably due to a decrease in the aspect ratio of the Fe nanowires, which results from the increase in their diameter. Furthermore, the crystal structure of the Fe nanowires may affect the coercivity.

  10. Magnetic Properties and Activity of Pt-Er/γ-Al2O3 Catalysts

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    A series of Pt-Er/γ-Al2O3 catalysts containing 0.5%(mass fraction) platinum and 0.05%-1.5% Er were prepared by impregnation of γ-Al2O3 supported with different concentrations of erbium chloride solution. The surface properties of the catalysts were studied by methods of temperature programmed reduction and temperature programmed desorption. The magnetic behavior of Pt-Er-γ-Al2O3 catalysts were studied with a Faraday magnetic balance and the results show that the addition of Er can affect the surface properties, the catalytic activities, and magnetic behavior of the reforming catalysts. It is found that there is a corresponding relationship between the susceptibility and selectivity of Pt-Er-γ-Al2O3 catalysts. The experimental results show that Er plays the role of electron promoter.

  11. Research on Catalytic Properties of Palladium Catalyst Prepared by Biological Reduction Method

    Institute of Scientific and Technical Information of China (English)

    Zhang Feng; Fu Jiquan

    2013-01-01

    This paper relates to highly dispersed supported Pd/MWCNTs and Pd/α-Al2O3 catalysts prepared by biological reduction method. The physico-chemical properties and the difference in catalytic activity of Pd catalysts prepared by bio-logical reduction method and chemical method, respectively, were investigated using XRD, TEM and speciifc surface char-acterization methods. The catalytic properties of catalysts were studied through activity evaluation means. The test results showed that the catalysts prepared by biological method were characteristic of small Pd nanoparticle size, good dispersion and low agglomeration, while possessing a high activity and stability in styrene hydrogenation reaction in comparison with catalysts prepared via the chemical method.

  12. Mixtures of Steel-Making Slag and Carbons as Catalyst for Microwave-Assisted Dry Reforming of CH4

    Institute of Scientific and Technical Information of China (English)

    Jose M. BERMUDEZ; Beatriz FIDALGO; Ana ARENILLAS; J. Angel MENENDEZ

    2012-01-01

    The use of steel-making slag as catalysts for microwave-assisted dry reforming of CH4 was studied.Two carbon materials (an activated carbon and a metallurgical coke),mixtures of the carbon materials and Fe-rich slag,and mixtures of the carbon materials and Ni/Al2O3 were tested as catalysts.The mixtures of slag with carbons gave rise to higher and steadier conversions than those achieved over the carbon materials alone.In addition,the use of the metallurgical coke mixed with metal-rich catalysts gave rise to remarkable results.Thus,no CH4 and CO2 conversions were achieved when coke was used alone,whereas high conversions were obtained when it was mixed with the metal-rich catalysts.

  13. POLYKETONE FROM ETHYLENE WITH CARBON MONOXIDE CATALYZED BY NOVEL CATALYST SYSTEMS BASED ON COPPER WITH BIDENTATE PHOSPHORUS CHELATING LIGANDS

    Institute of Scientific and Technical Information of China (English)

    Jun Huang; Feng-bo Li; Jin Zou; Guo-qing Yuan; Xiu-li Shi; Ding-sheng Yu

    2003-01-01

    Copolymerization of ethylene with carbon monoxide was performed with Cu catalyst systems. Novel catalyst systems based on Cu (Cu(CH3COO)2/ligand/acid) were firstly reported for the copolymerization of ethylene with carbon monoxide, in which the ligand was a bidentate phosphorus chelating ligand. The experimental results showed that this kind of Cu catalyst system exhibited high activity. When DPPP (1,3-bis(diphenylphosphine)propane) and CH3COOH were used catalyst system had the advantages of high stability and low cost.

  14. Hydrodeoxygenation of prairie cordgrass bio-oil over Ni based activated carbon synergistic catalysts combined with different metals.

    Science.gov (United States)

    Cheng, Shouyun; Wei, Lin; Zhao, Xianhui; Kadis, Ethan; Cao, Yuhe; Julson, James; Gu, Zhengrong

    2016-06-25

    Bio-oil can be upgraded through hydrodeoxygenation (HDO). Low-cost and effective catalysts are crucial for the HDO process. In this study, four inexpensive combinations of Ni based activated carbon synergistic catalysts including Ni/AC, Ni-Fe/AC, Ni-Mo/AC and Ni-Cu/AC were evaluated for HDO of prairie cordgrass (PCG) bio-oil. The tests were carried out in the autoclave under mild operating conditions with 500psig of H2 pressure and 350°C temperature. The catalysts were characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) and transmission electron microscope (TEM). The results show that all synergistic catalysts had significant improvements on the physicochemical properties (water content, pH, oxygen content, higher heating value and chemical compositions) of the upgraded PCG bio-oil. The higher heating value of the upgraded bio-oil (ranging from 29.65MJ/kg to 31.61MJ/kg) improved significantly in comparison with the raw bio-oil (11.33MJ/kg), while the oxygen content reduced to only 21.70-25.88% from 68.81% of the raw bio-oil. Compared to raw bio-oil (8.78% hydrocarbons and no alkyl-phenols), the Ni/AC catalysts produced the highest content of gasoline range hydrocarbons (C6-C12) at 32.63% in the upgraded bio-oil, while Ni-Mo/AC generated the upgraded bio-oil with the highest content of gasoline blending alkyl-phenols at 38.41%.

  15. Direct synthesis of dimethyl carbonate over rare earth oxide supported catalyst

    Institute of Scientific and Technical Information of China (English)

    JIANG Qi; CHENG Jiye; GAO Zhiqin

    2007-01-01

    Solid base catalysts for the direct synthesis of dimethyl carbonate (DMC)from carbon dioxide,methanol,and propylene oxide were prepared by loading KCl and K2CO3 on the surface of La2O3,Y2O31,CeO2 and Nd2O3.The catalysts were characterized by thermogravimetric analysis (TGA) and X-ray diffraction(XRD) techniques.The catalytic activities were efficiently influenced by the preparation conditions.The optimal loading amount of K2CO3 is 17.6%(mass)for KCl-K2CO3/Y2O3 and 22.2%for other catalysts.Supports affected the activity of catalyst.KCl-K2CO3/Nd2O3 exhibited the highest activity.The activity of KCl-K2CO3/Y2O3 increased wilh the increase of Calcination temperature in the range of 800℃-900℃.The formation of KYO2 Y3O4Cl or YOx species probably promoted the catalysts.

  16. Study of different nanostructured carbon supports for fuel cell catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Mirabile Gattia, Daniele; Antisari, Marco Vittori; Giorgi, Leonardo; Marazzi, Renzo; Montone, Amelia [Department of Physical Methods and Materials, ENEA, Research Centre of Casaccia, Via Anguillarese 301, 00123 Rome (Italy); Piscopiello, Emanuela [Department of Physical Methods and Materials, ENEA, Research Centre of Brindisi, Via Appia Km 702, 72100 Brindisi (Italy); Bellitto, Serafina; Licoccia, Silvia; Traversa, Enrico [Dipartimento di Scienze e Tecnologie Chimiche, Universita di Roma ' ' Tor Vergata' ' , Via della Ricerca Scientifica, 00133 Rome (Italy)

    2009-10-20

    Pt clusters were deposited by an impregnation process on three carbon supports: multi-wall carbon nanotubes (MWNT), single-wall carbon nanohorns (SWNH), and Vulcan XC-72 carbon black to investigate the effect of the carbon support structure on the possibility of reducing Pt loading on electrodes for direct methanol (DMFC) fuel cells without impairing performance. MWNT and SWNH were in-house synthesised by a DC and an AC arc discharge process between pure graphite electrodes, respectively. UV-vis spectrophotometry, scanning and transmission electron microscopy, X-ray diffraction, and cyclic voltammetry measurements were used to characterize the Pt particles deposited on the three carbon supports. A differential yield for Pt deposition, not strictly related to the surface area of the carbon support, was observed. SWNH showed the highest surface chemical activity toward Pt deposition. Pt deposited in different forms depending on the carbon support. Electrochemical characterizations showed that the Pt nanostructures deposited on MWNT are particularly efficient in the methanol oxidation reaction. (author)

  17. Zirconia/Titania Catalysts for Carbon Dioxide Utilisation

    OpenAIRE

    Al-Shafei, E.N.

    2015-01-01

    Reaction and conversion of CO2 to chemicals is a challenging area of research. The objective of this work is to study and investigate the use of mixed metal oxide Zr/Ti oxide and related catalysts for the conversion and utilisation of CO2. The first reaction studied was propane dehydrogenation using CO2 to produce propene. Then, the study extended to investigate the direct reaction of CO2 as whole molecule with methane, ethane, acetylene, ethylene and propane to synthesis carboxylic acids. ...

  18. Selective hydrogenation of citral over Au-based bimetallic catalysts in supercritical carbon dioxide

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    Selective hydrogenation of citral was investigated over Au-based bimetallic catalysts in the environmentally benign supercritical carbon dioxide (scCO2) medium.The catalytic performances were different in citral hydrogenation when Pd or Ru was mixed (physically and chemically) with Au.Compared with the corresponding monometallic catalyst,the total conversion and the selectivity to citronellal (CAL) were significantly enhanced over TiO2 supported Pd and Au bimetallic catalysts (physically and chemically mixed);however,the conversion and selectivity did not change when Ru was physically mixed with Au catalyst compared to the monometallic Ru/TiO2,and the chemically mixed Ru-Au/TiO2 catalyst did not show any activity.The effect of CO2 pressure on the conversion of citral and product selectivity was significantly different over the Au/TiO2,Pd-Au/TiO2,and Pd/TiO2 catalysts.It was assumed to be ascribed to the difference in the interactions between Au,Pd nanoparticles and CO2 under different CO2 pressures.

  19. Dinuclear Zinc Salen Catalysts for the Ring Opening Copolymerization of Epoxides and Carbon Dioxide or Anhydrides.

    Science.gov (United States)

    Thevenon, Arnaud; Garden, Jennifer A; White, Andrew J P; Williams, Charlotte K

    2015-12-21

    A series of four dizinc complexes coordinated by salen or salan ligands, derived from ortho-vanillin and bearing (±)-trans-1,2-diaminocyclohexane (L1) or 2,2-dimethyl-1,3-propanediamine (L2) backbones, is reported. The complexes are characterized using a combination of X-ray crystallography, multinuclear NMR, DOSY, and MALDI-TOF spectroscopies, and elemental analysis. The stability of the dinuclear complexes depends on the ligand structure, with the most stable complexes having imine substituents. The complexes are tested as catalysts for the ring-opening copolymerization (ROCOP) of CO2/cyclohexene oxide (CHO) and phthalic anhydride (PA)/CHO. All complexes are active, and the structure/activity relationships reveal that the complex having both L2 and imine substituents displays the highest activity. In the ROCOP of CO2/CHO its activity is equivalent to other metal salen catalysts (TOF = 44 h(-1) at a catalyst loading of 0.1 mol %, 30 bar of CO2, and 80 °C), while for the ROCOP of PA/CHO, its activity is slightly higher than other metal salen catalysts (TOF = 198 h(-1) at a catalyst loading of 1 mol % and 100 °C). Poly(ester-block-carbonate) polymers are also afforded using the most active catalyst by the one-pot terpolymerization of PA/CHO/CO2. PMID:26605983

  20. Synthesis of carbon nanotubes with and without catalyst particles

    Directory of Open Access Journals (Sweden)

    Cuniberti Gianaurelio

    2011-01-01

    Full Text Available Abstract The initial development of carbon nanotube synthesis revolved heavily around the use of 3d valence transition metals such as Fe, Ni, and Co. More recently, noble metals (e.g. Au and poor metals (e.g. In, Pb have been shown to also yield carbon nanotubes. In addition, various ceramics and semiconductors can serve as catalytic particles suitable for tube formation and in some cases hybrid metal/metal oxide systems are possible. All-carbon systems for carbon nanotube growth without any catalytic particles have also been demonstrated. These different growth systems are briefly examined in this article and serve to highlight the breadth of avenues available for carbon nanotube synthesis.

  1. Factors influencing electrochemical properties and performance of hydrocarbon based ionomer PEMFC catalyst layers

    OpenAIRE

    Astill, Toby Duncan

    2008-01-01

    This work investigated the properties of catalyst layers for proton exchange membrane fuel cells (PEMFC) that contained sulfonated poly(ether ether ketone) (SPEEK). A series of SPEEK polymers were prepared with varying ion exchange capacity (IEC) to test their oxygen mass transport properties, electrochemical kinetic parameters, proton conductivity, and water sorption characteristics. A simple method to fabricate catalyst layers containing SPEEK and polytetrafluoroethylene (PTFE) was develope...

  2. Highly active and stable platinum catalyst supported on porous carbon nanofibers for improved performance of PEMFC

    International Nuclear Information System (INIS)

    Porous carbon nanofibers (PCNFs) were used as the support to prepare platinum (Pt) catalyst (Pt/PCNFs) for proton exchange membrane fuel cell (PEMFC) applications. As a comparison, Pt supported on carbon black (Vulcan XC-72) (Pt/Vulcan) was also synthesized by the same ethylene glycol reduction method. Platinum was more uniformly deposited on PCNFs than that on the Vulcan XC-72. The electrocatalytic activity and stability of the resultant catalysts along with the commercial one (JM20) were investigated using cyclic voltammetry (CV) and linear sweep voltammetry (LSV) with a rotating disk electrode (RDE). The Pt/PCNFs exhibited much-enhanced electrocatalytic activity and stability compared with the Pt/Vulcan and JM20. The mass activity (at 0.80 V) of Pt/PCNFs is 2.6 times higher and 20% higher than that of Pt/Vulcan and JM20, respectively; the Pt/PCNFs retained about 50% of ECSA whereas JM20 and Pt/Vulcan kept only 25% and 5% of ECSA, respectively, even after 1000 cycles. Furthermore, the single cell performance of Pt/PCNFs was superior to that of Pt/Vulcan and even better than JM20 during high current densities. The cross-section of the membrane electrode assembly (MEA) showed that the Pt/PCNFs construct a loose three-dimensionally connected catalyst layer that is totally different from the tightly stacking catalyst layer composed of carbon black support. Thus, the mass transfer resistance is reduced and water drainage becomes easy when Pt/PCNFs were used as cathode catalyst. These results indicate PCNFs a promising candidate as catalyst supports for the enhancement of PEMFC performance

  3. Carbon-supported platinum alloy catalysts for phenol hydrogenation for making industrial chemicals

    Energy Technology Data Exchange (ETDEWEB)

    Srinivas, S.T.; Song, C.

    1999-07-01

    Phenol is available in large quantities in liquids derived from coal and biomass. Phenol hydrogenation is an industrially important reaction to produce cyclohexanone and cyclohexanol. Cyclohexane, cyclohexene and benzene are obtained as minor products in this reaction. Cyclohexanone is an important intermediate in the production of caprolactam for nylon 6 and cyclohexanol for adipic acid production. In USA, cyclohexanol and cyclohexanone are produced by benzene hydrogenation to cyclohexane over nickel or noble metal catalysts, followed by oxidation of cyclohexane to produce a mixture of cyclohexanol and cyclohexanone. Then cyclohexanol is dehydrogenated in the presence of Cu-Zn catalyst to cyclohexanone. Usually phenol hydrogenation is also carried out by using Ni catalyst in liquid phase. However, a direct single-step vapor phase hydrogenation of phenol to give cyclohexanone selectively is more advantageous in terms of energy savings and process economics, since processing is simplified and the endothermic step of cyclohexanol dehydrogenation can be avoided, as demonstrated by Montedipe and Johnson Matthey using promoted Pd/Al{sub 2}O{sub 3} catalyst. While it is not the purpose of this paper to dwell on the relative merits of these routes, it is necessary to mention that while using monometallic catalysts, generally the problem of catalyst deactivation of sintering as well as coking is frequently encountered. Addition and alloying of noble metal (e.g. Pt) with a second metal can result in a catalyst with better selectivity and activity in the reaction which is more resistant to deactivation. This paper presents the results on the single-step vapor phase hydrogenation of phenol over carbon-supported Pt-M (M=Cr, V, Zr) alloy catalysts to yield mainly cyclohexanone or cyclohexanol.

  4. USE OF CARBON CATALYSTS FOR OXIDATIVE DESTRUCTION OF WASTEWATERS

    Directory of Open Access Journals (Sweden)

    Svetlana S. Stavitskaya

    2007-06-01

    Full Text Available The paper considers a possibility of using the catalytic action of the carbonaceous adsorbents modified by different ways for the purification of various solutions, natural and wastewaters. It has been found that the oxidative destruction of organic (phenols, dyes, pesticides, etc. and inorganic (H2S contaminants in water solutions is considerably intensified in the presence of both ordinary activated carbons and especially, carbons with specially introduced catalytic additives. It is shown that the sewage treatment level is strongly affected by the amount and nature of a modifying agent introduced on the carbon surface.

  5. Studies on the Adsorption and Dissociation of Methane and Carbon Dioxide on Nickel Catalysts

    Institute of Scientific and Technical Information of China (English)

    Ling Qian; Zifeng Yan

    2002-01-01

    The adsorption and dissociation of methane and carbon dioxide for reforming on nickel catalysts were extensively investigated by TPSR, TPD, XPS and pulse reaction methods. These studies showed that the decomposition of methane results in the formation of at least three kinds of surface carbon species on supported nickel catalysts. Carbidic Cα, carbonaceous Cβ and carbidic clusters Cγ surface carbon species formed by the decomposition of methane demonstrated different surface mobility, thermal stability and reactivity. Carbidic Cα is a very active and important intermediate in carbon dioxide reforming with methane, and the carbidic clusters Cγ species might be the precursor of surface carbon deposition. The partially dehydrogenated Cβ species can react with H2 or CO2 to form CH4 or CO. On the other hand, it was proven that CO2 can be weakly adsorbed on supported nickel catalysts, and only one kind of CO2 adsorption state is formed. The interaction mechanism between the species dissociated from CH4 and CO2 during reforming was then hypothesized.

  6. EFFECT OF FOREIGN CARBON ON ACTIVITY OF METHANE COMBUSTION OVER SUPPORTED PALLADIUM CATALYSTS

    Institute of Scientific and Technical Information of China (English)

    Qi Caixia; An Lidun; Wang Hongli

    2001-01-01

    EDTA as precursor of carbon was introduced into Pd(NO3)2 catalysts supported on γ-Al2O3 or 5%MgO/γ-Al2O3. Two kinds of samples,denoted as Pd(NO3)2/[support+EDTA] and [Pd(NO3)2/support]+EDTA, were prepared by changing sequence of impregnating EDTA to the supports. After only being dried they were tested for methane combustion. XPS analyses to the samples at different stages of testing reaction were performed. It was found that the Pd(NO3)2 catalysts became more inactive due to the introduction of EDTA. EDTA in the catalysts was naturally in situ oxidized,partially became into CO2 and escaped, partially coked and deposited on palladium and support with temperature increasing in oxygen-rich atmosphere.Formation of Pd-C solid solution was also confirmed during the reaction. It can be suggested that foreign carbon, in spite of its any existing forms and position in catalysts, inhibits methane combustion largely. The role of carbon on morphological change of palladium during methane combustion was also discussed.

  7. Carbon nanotubes/tin oxide nanocomposite-supported Pt catalysts for methanol electro-oxidation.

    Science.gov (United States)

    Li, Xingwei; Wei, Jiadi; Chai, Yuzheng; Zhang, Shuo

    2015-07-15

    Carbon nanotubes/tin oxide nanocomposite (MWCNTs-SnO2) was obtained via the hydrolysis of SnCl4 in the presence of multi-walled carbon nanotubes (MWCNTs) and subsequent calcinations. And carbon nanotubes/tin oxide nanocomposite-supported Pt catalysts (Pt/MWCNTs-SnO2) were prepared by in-situ liquid phase reduction using H2PtCl6 as a metal precursor. As-prepared catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM), and their catalytic performances were evaluated by chronoamperometry (CA) and cyclic voltammetry (CV). Desirable catalytic performance for methanol electro-oxidation was observed with a reduced size and an improved dispersion of Pt catalysts on the MWCNTs-SnO2 nanocomposite. The calcination temperature of MWCNTs-SnO2 nanocomposite was a key factor for controlling the catalytic performance of Pt/MWCNTs-SnO2 catalysts. PMID:25801135

  8. Kinetics of wet peroxide oxidation of phenol with a gold/activated carbon catalyst

    OpenAIRE

    Domínguez, Carmen M.; Quintanilla, Asunción; Casas, José Antonio; Rodríguez, Juan José

    2014-01-01

    Gold nanoparticles supported on activated carbon (Au/AC) have been tested in catalytic wet peroxide oxidation using phenol as target pollutant. In the current work, the effect of several operating conditions, including initial pH (3.5–10.5), catalyst load (0–6 g/L), initial phenol concentration (0.1–5 g/L), hydrogen peroxide dose (4–100% of the theoretical stoichiometric amount) and reaction temperature (50–80 °C) has been investigated. The results show that the Au/AC catalyst would be useful...

  9. Towards Green Cyclic Carbonate Synthesis : Heterogeneous and Homogeneous Catalyst Development

    OpenAIRE

    Stewart, J A

    2015-01-01

    This PhD research serves to implement both known and novel catalytic systems for the purpose of cyclic carbonate synthesis from biomass-derived substrates. Such products have been earmarked as potential monomers for non-isocyanate polyurethanes (NIPUs), amongst other uses. Particular attention has been placed on operating under the guidance of the 12 principles of Green Chemistry as posited by Anastas et al. Following an in depth literature discussion of catalytic cyclic carbonate synthesis i...

  10. Carbon and glass hierarchical fibers: Influence of carbon nanotubes on tensile, flexural and impact properties of short fiber reinforced composites

    International Nuclear Information System (INIS)

    Highlights: ► Dense CNT were grown on carbon fiber and glass fiber by use of floating catalyst CVD method. ► CNT showed different growing mechanism on carbon and glass fiber. ► Short fiber-CNT-composites showed enhanced mechanical properties. ► CNT coating enhanced fiber–matrix interaction and acted as additional reinforcement. -- Abstract: Dense carbon nanotubes (CNTs) were grown uniformly on the surface of carbon fibers and glass fibers to create hierarchical fibers by use of floating catalyst chemical vapor deposition. Morphologies of the CNTs were investigated using scanning electronic microscope (SEM) and transmission electron microscope (TEM). Larger diameter dimension and distinct growing mechanism of nanotubes on glass fiber were revealed. Short carbon and glass fiber reinforced polypropylene composites were fabricated using the hierarchical fibers and compared with composites made using neat fibers. Tensile, flexural and impact properties of the composites were measured, which showed evident enhancement in all mechanical properties compared to neat short fiber composites. SEM micrographs of composite fracture surface demonstrated improved adhesion between CNT-coated fiber and the matrix. The enhanced mechanical properties of short fiber composites was attributed to the synergistic effects of CNTs in improving fiber–matrix interfacial properties as well as the CNTs acting as supplemental reinforcement in short fiber-composites.

  11. One-pot Synthesis of Dimethyl Carbonate in the Presence of a Two-component Catalyst

    Institute of Scientific and Technical Information of China (English)

    CHEN Xiu-zhi; HU Chang-wen; GAO Zhi-ming

    2005-01-01

    The one-pot synthesis of dimethyl carbonate (DMC) with co-production of propy-lene carbonate(PC) and propylene glycol(PG) from propylene oxide( PO), carbon dioxide and methanol as the starting materials was investigated.The catalyst adopted here was a mixture of tetrabutyl ammonium bromide and sodium methoxide. It was found that under the reaction conditions of t = 150 ℃, p =3-4 MPa and 2 h, the PO conversion could reach 100%, the DMC,PC and the PG selectivities were 49.7%, 42.7% and 49. 8%, respectively, and the selectivity of by-products was below 10%.

  12. A trimodal porous carbon as an effective catalyst for hydrogen production by methane decomposition.

    Science.gov (United States)

    Shen, Yi; Lua, Aik Chong

    2016-01-15

    A new type of porous carbon with an interconnected trimodal pore system is synthesized by a nanocasting method using nanoparticulated bimodal micro-mesoporous silica particles as the template. The synthesized template and carbon material are characterized using transmission electron microscopy (TEM), field emission electron scanning microscopy (FESEM) and nitrogen adsorption-desorption test. The synthesized carbon material has an extremely high surface area, a large pore volume and an interconnected pore structure, which could provide abundant active sites and space for chemical reactions and minimize the diffusion resistance of the reactants. The resulting carbon is used as the catalyst for hydrogen production by the thermal decomposition of methane. The catalytic results show that the as-synthesized carbon in this study produces much higher methane conversion and hydrogen yield than the commercial carbon materials. PMID:26433477

  13. Direct synthesis of diphenyl carbonate over heterogeneous catalyst:effects of structure of substituted perovskite carrier on the catalyst activities

    Institute of Scientific and Technical Information of China (English)

    WU Guangwen; WU Yuxin; MA Peisheng; JIN Fang; ZHANG Guangxu; LI Dinghuo; WANG Cunwen

    2007-01-01

    The perovskite-type compound LaMnO3 was substituted for the part of La in position A and for the part of Mn in position B by citrate method.The phases were detected by X-ray diffraction.Powder morphologies were scanned by scanning electron microscopy.The valence of atoms was determined by X-ray photoelectron spectroscopy.It was found that the perovskite can form crystal defect and increase the proportion of high valence B element by doping.Active component Pd was loaded on various perovskite supports for synthesis of diphenyl carbonate.The results showed that the activities of catalysts in which supports have crystal defect by substitution were higher.It can be concluded that perovskite with defect structure by doping could lead to the formation of oxygen vacancy where the lattice oxygen became exchangeable with the oxygen gas.Also,this improved the redox process of the carrier by transferring electrons and activities of catalysts.

  14. Influence of Ni Catalyst Layer and TiN Diffusion Barrier on Carbon Nanotube Growth Rate

    Directory of Open Access Journals (Sweden)

    Mérel Philippe

    2010-01-01

    Full Text Available Abstract Dense, vertically aligned multiwall carbon nanotubes were synthesized on TiN electrode layers for infrared sensing applications. Microwave plasma-enhanced chemical vapor deposition and Ni catalyst were used for the nanotubes synthesis. The resultant nanotubes were characterized by SEM, AFM, and TEM. Since the length of the nanotubes influences sensor characteristics, we study in details the effects of changing Ni and TiN thickness on the physical properties of the nanotubes. In this paper, we report the observation of a threshold Ni thickness of about 4 nm, when the average CNT growth rate switches from an increasing to a decreasing function of increasing Ni thickness, for a process temperature of 700°C. This behavior is likely related to a transition in the growth mode from a predominantly “base growth” to that of a “tip growth.” For Ni layer greater than 9 nm the growth rate, as well as the CNT diameter, variations become insignificant. We have also observed that a TiN barrier layer appears to favor the growth of thinner CNTs compared to a SiO2 layer.

  15. On the stability of carbon nanotube and titania nanowire based catalyst materials:from synthesis to applications

    OpenAIRE

    Rautio, A.-R. (Anne-Riikka)

    2016-01-01

    Abstract Degradation of the support and sintering of catalyst nanoparticles inherently leads to a loss of functionality of catalyst materials in converters and sensors. Malfunction in such devices may lead to serious economic and environmental damage. The quest for novel and sustainable catalyst materials with better durability is thus ongoing. In this thesis, one-dimensional nanomaterials such as carbon nanotubes and titanium dioxide nanowires are studied and compared to their convention...

  16. High efficient acetalization of carbonyl compounds with diols catalyzed by novel carbon-based solid strong acid catalyst

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    The novel carbon-based acid catalyst has been applied to catalyzing the acetalization and ketalization. The results showed that the catalyst was very efficient with the average yield over 93%. The novel heterogeneous catalyst has the advantages of high activity, wide applicability even to 7-membered ring acetals, strikingly simple workup procedure, non-pollution, and reusability, which will contribute to the green process greatly.

  17. Synthesis of a Novel Carbon Based Acid Catalyst and Its Catalytic Activity for the Acetalization and Ketalization

    Institute of Scientific and Technical Information of China (English)

    LIANG Xue-Zheng; GAO Shan; CHEN Wen-Ping; WANG Wen-Juan; YANG Jian-Guo

    2007-01-01

    A novel carbon based strong solid acid catalyst has been synthesized successfully.The catalytic activity for acetalization and ketalization was investigated.The results showed that the novel catalyst was very efficient with the average yield over 92%.The novel heterogeneous catalyst also has the advantages of high activity,wide applicability even to the preparation of 7 membered ring acetals and ketals,strikingly simple workup procedure,non-pollution and reusability,which will contribute to the green process greatly.

  18. Influence of carbon nanofiber properties as electrocatalyst support on the electrochemical performance for PEM fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Sebastian, D.; Suelves, I.; Moliner, R.; Lazaro, M.J. [Instituto de Carboquimica (CSIC), Energy and Environment, C/Miguel Luesma Castan 4, 50018 Zaragoza (Spain); Calderon, J.C.; Gonzalez-Exposito, J.A.; Pastor, E. [Universidad de La Laguna, Dpto de Quimica-Fisica, Avda. Astrofisico Francisco Sanchez s/n, 38071 La Laguna, Tenerife (Spain); Martinez-Huerta, M.V. [Instituto de Catalisis y Petroleoquimica (CSIC), C/Marie Curie 2, 28049 Madrid (Spain)

    2010-09-15

    Novel carbonaceous supports for electrocatalysts are being investigated to improve the performance of polymer electrolyte fuel cells. Within several supports, carbon nanofibers blend two properties that rarely coexist in a material: a high mesoporosity and a high electrical conductivity, due to their particular structure. Carbon nanofibers have been obtained by catalytic decomposition of methane, optimizing growth conditions to obtain carbon supports with different properties. Subsequently, the surface chemistry has been modified by an oxidation treatment, in order to create oxygen surface groups of different nature that have been observed to be necessary to obtain a higher performance of the electrocatalyst. Platinum has then been supported on the as-prepared carbon nanofibers by different deposition methods and the obtained catalysts have been studied by different electrochemical techniques. The influence of carbon nanofibers properties and functionalization on the electrochemical behavior of the electrocatalysts has been studied and discussed, obtaining higher performances than commercial electrocatalysts with the highest electrical conductive carbon nanofibers as support. (author)

  19. Development of niobium-promoted cobalt catalysts on carbon nanotubes for Fischer-Tropsch synthesis

    Institute of Scientific and Technical Information of China (English)

    Sardar Ali; Noor Asmawati Mohd Zabidi; Duvvuri Subbarao

    2011-01-01

    Cobalt-based catalysts were prepared by a wet impregnation method on carbon nanotubes (CNTs) support and promoted with niobium.Samples were characterized by nitrogen adsorption,TEM,XRD,TPR,TPO and H2-TPD.Addition of niobium increased the dispersion of cobalt but decreased the catalysts reducibility.Fischer-Tropsch synthesis (FTS) was carried out in a fixed-bed microreactor at 543 K,1 atm and H2/CO =2 for 5 h.Addition of niobium enhanced the C5+ hydrocarbons selectivity by 39% and reduced methane selectivity by 59%.These effects were more pronounced for 0.04%Nb/Co/CNTs catalyst,compared with those observed for other niobium compositions.

  20. Direct synthesis of dimethyl carbonate from methanol and carbon dioxide over CeO2(X)-ZnO(1-X) nano-catalysts.

    Science.gov (United States)

    Kang, Ki Hyuk; Joe, Wangrae; Lee, Chang Hoon; Kim, Mieock; Kim, Dong Baek; Jang, Boknam; Song, In Kyu

    2013-12-01

    CeO2(X)-ZnO(1-X) (X = 0, 0.1, 0.3, 0.5, 0.7, 0.9, and 1.0) nano-catalysts were prepared by a co-precipitation method with a variation of CeO2 content (X, mol%), and they were applied to the direct synthesis of dimethyl carbonate from methanol and carbon dioxide. Successful formation of CeO2(X)-ZnO(1-X) nano-catalysts was well confirmed by XRD analysis. The amount of DMC produced over CeO2(X)-ZnO(1-X) catalysts exhibited a volcano-shaped curve with respect to CeO2 content. Acidity and basicity of CeO2(X)-ZnO(1-X) nano-catalysts were measured by NH3-TPD and CO2-TPD experiments, respectively, to elucidate the effect of acidity and basicity on the catalytic performance in the reaction. It was revealed that the catalytic performance of CeO2(X)-ZnO(1-X) nano-catalysts was closely related to the acidity and basicity of the catalysts. Amount of dimethyl carbonate increased with increasing both acidity and basicity of the catalysts. Among the catalysts tested, CeO2(0.7)-ZnO(0.3) with the largest acidity and basicity showed the best catalytic performance in the direct synthesis of dimethyl carbonate from methanol and carbon dioxide. PMID:24266202

  1. Carbon felt supported carbon nanotubes catalysts composite electrode for vanadium redox flow battery application

    Science.gov (United States)

    Wei, Guanjie; Jia, Chuankun; Liu, Jianguo; Yan, Chuanwei

    2012-12-01

    A modified electrode for vanadium redox flow battery (VRFB) has been developed in this paper. The electrode is based on a traditional carbon felt (CF) grafted with the short-carboxylic multi-walled carbon nanotubes (MWCNTs). The microstructure and electrochemical property of the modified electrode as well as the performance of the VRFB single cell with it have been characterized. The results show that the MWCNTs are evenly dispersed and adhere to the surface of carbon fibres in the CF. The electrochemical activities of the modified CF electrode have been improved dramatically and the reversibility of the VO2+/VO2+ and V3+/V2+ redox couples increased greatly. The VRFB single cell with the modified CF exhibits higher coulombic efficiency (93.9%) and energy efficiency (82.0%) than that with the pristine CF. The SEM analysis shows that the MWCNTs still cohere with carbon fibres after charge and discharge test, indicating the stability of the MWCNTs in flowing electrolyte. Therefore, the composite electrode presents considerable potential for the commercial application of CF in VRFB.

  2. N-doped mesoporous carbons supported palladium catalysts prepared from chitosan/silica/palladium gel beads.

    Science.gov (United States)

    Zeng, Minfeng; Wang, Yudong; Liu, Qi; Yuan, Xia; Feng, Ruokun; Yang, Zhen; Qi, Chenze

    2016-08-01

    In this study, a heterogeneous catalyst including palladium nanoparticles supported on nitrogen-doped mesoporous carbon (Pd@N-C) is synthesized from palladium salts as palladium precursor, colloidal silica as template, and chitosan as carbon source. N2 sorption isotherm results show that the prepared Pd@N-C had a high BET surface area (640m(2)g(-1)) with large porosity. The prepared Pd@N-C is high nitrogen-rich as characterized with element analysis. X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HR-TEM), and Raman spectroscopy characterization of the catalyst shows that the palladium species with different chemical states are well dispersed on the nitrogen-containing mesoporous carbon. The Pd@N-C is high active and shows excellent stability as applied in Heck coupling reactions. This work supplies a successful method to prepare Pd heterogeneous catalysts with high performance from bulk biopolymer/Pd to high porous nitrogen-doped carbon supported palladium catalytic materials. PMID:27155234

  3. Preparation of catalyst for a polymer electrolyte fuel cell using a novel spherical carbon support

    Energy Technology Data Exchange (ETDEWEB)

    Eguchi, Mika; Okubo, Atsuhiko; Kobayashi, Yoshio [Department of Biomolecular Functional Engineering, Faculty of Engineering, Ibaraki University, 4-12-1, Nakanarusawa, Hitachi, Ibaraki 316-8511 (Japan); Yamamoto, Shun [Material and Biological Sciences, Graduate School of Science and Engineering, Faculty of Engineering, Ibaraki University, 4-12-1, Nakanarusawa, Hitachi, Ibaraki 316-8511 (Japan); Kikuchi, Mayuko; Nishitani-Gamo, Mikka [Department of Applied Chemistry, Faculty of Engineering, Toyo University, 2100 Kujirai, Kawagoe, Saitama 350-8585 (Japan); Uno, Katsuhiro [Department of Media and Telecommunications Engineering, Faculty of Engineering, Ibaraki University, 4-12-1, Nakanarusawa, Hitachi, Ibaraki 316-8511 (Japan); Ando, Toshihiro [National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)

    2010-09-15

    In this study, the support Pt catalyst was supported by a novel spherical carbon using a convenient technique. Two different preparation methods utilizing a nanocolloidal solution method without heat treatment were developed (methods 1 and 2). The scanning electron microscope (SEM) and transmission electron microscope (TEM) observations showed that the Pt nanoparticles (particle size) were supported, with higher dispersion being achieved with method 2 than method 1. The peak of the Pt metal was confirmed from the X-ray diffraction (XRD) measurement. Based on the inductively coupled plasma mass spectrometry (ICP-MS) measurements, Pt loading was 19.5 wt.% in method 1 and approximately 50 wt.% in method 2. The Pt specific surface area of the Pt/novel spherical carbon catalyst calculated from the cyclic voltammetry (CV) measurement result was larger than that of the commercially available Pt/Ketjen catalyst. These results indicated that the Pt nanoparticles were supported in high dispersion without heat treatment using novel spherical carbon as a carbon support. (author)

  4. Carbon Aerogel-Supported Pt Catalysts for the Hydrogenolysis and Isomerization of n-Butane: Influence of the Carbonization Temperature of the Support and Pt Particle Size

    Directory of Open Access Journals (Sweden)

    Marta B. Dawidziuk

    2012-10-01

    Full Text Available Carbon aerogels prepared at different carbonization temperatures and with varying mesopore volumes were used as supports for Pt catalysts to study the n-C4H10/H2 reaction. Mean Pt particle size depended on the mesopore volume of the support, showing a linear decrease when the mesopore volume increased. The turnover frequency (TOF for hydrogenolysis was much higher than for isomerization in catalysts supported on carbon aerogels obtained at 900–950 °C. However, both TOF values were similar in catalysts supported on the carbon aerogel obtained at 500 °C. TOF for hydrogenolysis and isomerization were related to the mean Pt particle size in catalysts supported on carbon aerogels obtained at 900–950 °C. In addition, both reactions showed a compensation effect between the activation energy and pre-exponential factor, indicating that they have the same intermediate, i.e., the chemisorbed dehydrogenated alkane.

  5. Tuning field emission properties of boron nanocones with catalyst concentration

    Institute of Scientific and Technical Information of China (English)

    Li Chen; Tian Yuan; Wang Deng-Ke; Shi Xue-Zhao; Hui Chao; Shen Cheng-Min; Gao Hong-Jun

    2011-01-01

    Single crystalline boron nanocones are prepared by using a simple spin spread method in which Fe3O4 nanoparticles are pre-manipulated on Si(111) to form catalyst patterns of different densities. The density of boron nanocones can be tuned by changing the concentration of catalyst nanoparticles. High-resolution transmission electron microscopy analysis shows that the boron nanocone has a β-tetragonal structure with good crystallization. The field emission behaviour is optimal when the spacing distance is close to the nanocone length, which indicates that this simple spin spread method has great potential applications in electron emission nanodevices.

  6. Study of Carbon Nanotube Supported Co-Mo Selective Hydrodesulphurization Catalysts for Fluid Catalytic Cracking Gasoline

    Institute of Scientific and Technical Information of China (English)

    Wenkui Yin; Mei Li; Hongyan Shang; Chenguang Liu; Fei Wei

    2005-01-01

    In this paper,carbon nanotube supported Co-Mo catalysts for selective hydrodesulphurization (HDS) of fluid catalytic cracking (FCC) gasoline were studied,using di-isobutylene,cyclohexene,1-octene and thiophene as model compounds to simulate FCC gasoline. The results show that the Co-Mo/CNT has very high HDS activity and HDS/hydrogenation selectivity comparing with the Co-Mo/γ-Al2O3 and Co-Mo/AC catalyst systems. The saturation ratio of cyclohexene was lower than 50%,and the saturation ratio of 1,3-di-isobutylene lower than 60% for the Co-Mo/CNT catalysts. Co/Mo atomic ratio was found to be one of the most important key factors in influencing the hydrogenation selectivity and HDS activity,and the most suitable Co/Mo atomic ratio was 0.4. Co/CNT and Mo/CNT mono-metallic catalysts showed lower HDS activity and selectivity than the Co-Mo/CNT bi-metallic catalysts.

  7. Carbon-Supported bimetallic Pd-Fe catalysts for vapor-phase hydrodeoxygenation of guaiacol

    Energy Technology Data Exchange (ETDEWEB)

    Sun, Junming; Karim, Ayman M.; Zhang, He; Kovarik, Libor; Li, Xiaohong S.; Hensley, Alyssa; McEwen, Jean-Sabin; Wang, Yong

    2013-10-01

    Abstract Carbon supported metal catalysts (Cu/C, Fe/C, Pd/C, Pt/C, PdFe/C and Ru/C) have been prepared, characterized and tested for vapor-phase hydrodeoxygenation (HDO) of guaiacol (GUA) at atmospheric pressure. Phenol was the major intermediate on all catalysts. Over the noble metal catalysts saturation of the aromatic ring was the major pathway observed at low temperature (250 °C), forming predominantly cyclohexanone and cyclohexanol. Substantial ring opening reaction was observed on Pt/C and Ru/C at higher reaction temperatures (e.g., 350 °C). Base metal catalysts, especially Fe/C, were found to exhibit high HDO activity without ring-saturation or ring-opening with the main products being benzene, phenol along with small amounts of cresol, toluene and trimethylbenzene (TMB). A substantial enhancement in HDO activity was observed on the PdFe/C catalysts. Compared with Fe/C, the yield to oxygen-free aromatic products (i.e., benzene/toluene/TMB) on PdFe/C increased by a factor of four at 350 °C, and by approximately a factor of two (83.2% versus 43.3%) at 450 °C. The enhanced activity of PdFe/C is attributed to the formation of PdFe alloy as evidenced by STEM, EDS and TPR.

  8. Towards Green Cyclic Carbonate Synthesis : Heterogeneous and Homogeneous Catalyst Development

    NARCIS (Netherlands)

    Stewart, J.A.

    2015-01-01

    This PhD research serves to implement both known and novel catalytic systems for the purpose of cyclic carbonate synthesis from biomass-derived substrates. Such products have been earmarked as potential monomers for non-isocyanate polyurethanes (NIPUs), amongst other uses. Particular attention has b

  9. Vapor Phase Hydrogenation of Nitrobenzene to Aniline Over Carbon Supported Ruthenium Catalysts.

    Science.gov (United States)

    Srikanth, Chakravartula S; Kumar, Vanama Pavan; Viswanadham, Balaga; Srikanth, Amirineni; Chary, Komandur V R

    2015-07-01

    A series of Ru/Carbon catalysts (0.5-6.0 wt%) were prepared by impregnation method. The catalysts were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), CO-chemisorption, surface area and pore-size distribution measurements. The catalytic activities were evaluated for the vapor phase hydrogenation of nitrobenzene. The dispersion measured by CO-uptake values suggests that a decrease of dispersion is observed with increasing Ru loading on carbon support. These findings are well supported by the crystallite size measured from XRD measurements. XPS study reveals the formation of Ru0 after reduction at 573 K for 3 h. The catalysts exhibit high conversion/selectivity at 4.5 wt% Ru loading during hydrogenation reaction. The particle size measured from CO-chemisorption and TEM analysis are related to the TOF during the hydrogenation reaction. Ru/C catalysts are found to show higher conversion/selectivities during hydrogenation of nitrobenzene to aniline. PMID:26373150

  10. Cationic organobismuth complex as an effective catalyst for conversion of CO2 into cyclic carbonates

    Institute of Scientific and Technical Information of China (English)

    Xiaowen ZHANG; Weili DAI; Shuangfeng YIN; Shenglian LUO; Chak-Tong AU

    2009-01-01

    In order to achieve high-efficiency conversion of CO2 into valuable chemicals, and to exploit new appli-cations of organobismuth compounds, cationic organo-bismuth complex with 5,6,7,12-tetrahydrodibenz[c,f] [ 1,5 ]azabismocine framework was examined for the first time for the coupling of CO2 into cyclic carbonates, using ter-minal epoxides as substrates and tetrabutylammonium halide as co-catalyst in a solvent-free environment under mild conditions. It is shown that the catalyst exhibited high activity and selectivity for the coupling reaction of CO2 with a wide range of terminal epoxide. The selectivity of propylene carbonates could reach 100%, and the max-imum turnover frequency was up to 10740 h-1 at 120℃ and 3 MPa CO2 pressure when tetrabutylammonium iod-ide was used as co-catalyst. Moreover, the catalyst is environment friendly, resistant to air and water, and can be readily reused and recycled without any loss of activity,demonstrating a potential in industrial application.

  11. Towards stable catalysts by controlling collective properties of supported metal nanoparticles

    Science.gov (United States)

    Prieto, Gonzalo; Zečević, Jovana; Friedrich, Heiner; de Jong, Krijn P.; de Jongh, Petra E.

    2013-01-01

    Supported metal nanoparticles play a pivotal role in areas such as nanoelectronics, energy storage/conversion and as catalysts for the sustainable production of fuels and chemicals. However, the tendency of nanoparticles to grow into larger crystallites is an impediment for stable performance. Exemplarily, loss of active surface area by metal particle growth is a major cause of deactivation for supported catalysts. In specific cases particle growth might be mitigated by tuning the properties of individual nanoparticles, such as size, composition and interaction with the support. Here we present an alternative strategy based on control over collective properties, revealing the pronounced impact of the three-dimensional nanospatial distribution of metal particles on catalyst stability. We employ silica-supported copper nanoparticles as catalysts for methanol synthesis as a showcase. Achieving near-maximum interparticle spacings, as accessed quantitatively by electron tomography, slows down deactivation up to an order of magnitude compared with a catalyst with a non-uniform nanoparticle distribution, or a reference Cu/ZnO/Al2O3 catalyst. Our approach paves the way towards the rational design of practically relevant catalysts and other nanomaterials with enhanced stability and functionality, for applications such as sensors, gas storage, batteries and solar fuel production.

  12. Improving the durability of methanol oxidation reaction electro-catalysts through the modification of carbon architectures

    Science.gov (United States)

    Wood, Kevin N.

    Carbon materials represent one of the largest areas of studied research today, having integrated applications stretching from energy production and storage to medical use and far beyond. One of these many intriguing applications is fuel cells, which offers the promise of clean electricity through a direct electrochemical energy conversion process. Unfortunately, at the present time the cost per watt-hour produced by fuel cells is more expensive than conventional methods of energy production/storage (i.e. combustion engines, batteries, etc.). Under the umbrella of fuel cell systems, methanol is a promising fuel source because of its high energy density and convenience of direct liquid fuel operation. In this field, recent advancements are bringing direct methanol fuel cells (DMFCs) closer to commercial viability. However, just as in other fuel cell systems, further improvements are greatly needed, particularly in the area of catalyst durability. This need for improved durability has led to increased research activity focused on improving catalyst stability and utilization. This thesis explores one of the most promising areas of enhancing catalyst-support interactions; namely, modification of carbon support architectures. Through the use of heteroatom modifiers, such as nitrogen, fuel cell support systems can be enhanced in such a way as to improve metal nucleation and growth, catalyst durability and catalytic activity. To this end, this thesis employs advanced characterization techniques to study the changes in catalyst particle morphology before and after nitrogen modification of the support structure. These results clearly show the beneficial effects of nitrogen moieties on carbon structures and help elucidate the effects of nitrogen on the stability of supported catalytic nanoparticles systems. Similarly, the novel concept of post-modifying commercially available supported catalysts with nitrogen ion implantation gives further insight into the behavior of

  13. K2O对合成 DMC用 Cu-Ni/V2O5-SiO2催化剂性能的影响%Effect of K2O on Properties of Cu-Ni/V2O5-SiO2 Catalyst for the Synthesis of Dimethyl Carbonate

    Institute of Scientific and Technical Information of China (English)

    黎汉生; 钟顺和; 王建伟; 肖秀芬

    2001-01-01

    V2O5-SiO2(VSiO) supported Cu-Ni-K2O catalysts for the synthesis of dimethyl carbonate were prepared using isovolumic impregnation. Based on TPR,TPD, IR and micro-reactor techniques, the effect of K2O on the adsorption and reaction of CO2 and CH3OH on the catalyst were characterized. The results show that addition of K2O exerts obvious influence on the charge distribution of the active sites on Cu-Ni/VSiO catalyst,increases the intensities of CO2 horizontal adsorption state, while that of the dissociation state of methanol descends. When the ratio of K is above 15 % , K2CO3 is formed on the catalyst. Moreover,the main reaction products of CO2 and CH3OH on Cu-Ni-K2O/VSiO catalyst are still DMC, H2O, CO and CH2O,and with the addition of K2O, the conversion of reactants rise, but the selectivity of by-products decreases.

  14. Palladium on Nitrogen-Doped Mesoporous Carbon: A Bifunctional Catalyst for Formate-Based, Carbon-Neutral Hydrogen Storage.

    Science.gov (United States)

    Wang, Fanan; Xu, Jinming; Shao, Xianzhao; Su, Xiong; Huang, Yanqiang; Zhang, Tao

    2016-02-01

    The lack of safe, efficient, and economical hydrogen storage technologies is a hindrance to the realization of the hydrogen economy. Reported herein is a reversible formate-based carbon-neutral hydrogen storage system that is established over a novel catalyst comprising palladium nanoparticles supported on nitrogen-doped mesoporous carbon. The support was fabricated by a hard template method and nitridated under a flow of ammonia. Detailed analyses demonstrate that this bicarbonate/formate redox equilibrium is promoted by the cooperative role of the doped nitrogen functionalities and the well-dispersed, electron-enriched palladium nanoparticles. PMID:26763714

  15. Palladium on Nitrogen-Doped Mesoporous Carbon: A Bifunctional Catalyst for Formate-Based, Carbon-Neutral Hydrogen Storage.

    Science.gov (United States)

    Wang, Fanan; Xu, Jinming; Shao, Xianzhao; Su, Xiong; Huang, Yanqiang; Zhang, Tao

    2016-02-01

    The lack of safe, efficient, and economical hydrogen storage technologies is a hindrance to the realization of the hydrogen economy. Reported herein is a reversible formate-based carbon-neutral hydrogen storage system that is established over a novel catalyst comprising palladium nanoparticles supported on nitrogen-doped mesoporous carbon. The support was fabricated by a hard template method and nitridated under a flow of ammonia. Detailed analyses demonstrate that this bicarbonate/formate redox equilibrium is promoted by the cooperative role of the doped nitrogen functionalities and the well-dispersed, electron-enriched palladium nanoparticles.

  16. Efficient strategy to Cu/Si catalyst into vertically aligned carbon nanotubes with bamboo shape by CVD technique

    Indian Academy of Sciences (India)

    V MOHANA KRISHNA; T SOMANATHAN

    2016-08-01

    Bamboo-shaped vertically aligned carbon nanotubes (bs-VACNTs) were fabricated on Cu/Si catalyst by chemical vapour deposition (CVD) technique under the atmospheric pressure. The catalytic material (Cu/Si) playeda vital role in attaining bs-VACNTs, which is synthesized by drop cast method in a cost-effective manner. Using this catalytic support, we have achieved the tip growth bs-VACNTs at low temperature with well graphitization. The as-grown carbon material was then characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive X-ray spectroscopy (EDX) analyzer, high-resolution transmission electron microscope (HRTEM) and Raman spectroscopy. XRD technique confirms the formation of hexagonal graphitic carbon planes of carbon nanotubes (CNTs). The surface morphology of the material was characterized by SEM, which clearly infervertically aligned CNTs. The nature, diameter and crystallinity were noticed by HRTEM and Raman spectroscopy, respectively. Further, we have also studied the electrochemical properties of the bs-VACNTs and it seems to be proved as highly electroconductive when compared to multi-walled carbon nanotubes (MWCNTs).

  17. High-performance oxygen reduction catalyst derived from porous, nitrogen-doped carbon nanosheets

    Science.gov (United States)

    Wang, Hao; Chen, Kai; Cao, Yingjie; Zhu, Juntong; Jiang, Yining; Feng, Lai; Dai, Xiao; Zou, Guifu

    2016-10-01

    A facile, self-foaming strategy is reported to synthesize porous, nitrogen-doped carbon nanosheets (N-CNSs) as a metal-free electrocatalyst for oxygen reduction reaction (ORR). Benefiting from the synergistic functions of N-induced active sites, a highly specific surface area and continuous structure, the optimal N-CNS catalyst exhibits Pt-like ORR activity (positive onset potential of ˜0 V versus Ag/AgCl and limiting current density of 5 mA cm-2) through a four-electron transfer process in alkaline media with excellent cycle stability and methanol tolerance. This work not only provides a promising metal-free ORR catalyst but also opens up a new path for designing carbon-based materials towards broad applications.

  18. Microwave-assisted synthesis of carbon-supported carbides catalysts for hydrous hydrazine decomposition

    Science.gov (United States)

    Mnatsakanyan, Raman; Zhurnachyan, Alina R.; Matyshak, Valery A.; Manukyan, Khachatur V.; Mukasyan, Alexander S.

    2016-09-01

    Microwave-assisted synthesis of carbon-supported Mo2C and WC nanomaterials was studied. Two different routes were utilized to prepare MoO3 (WO3) - C precursors that were then subjected to microwave irradiation in an inert atmosphere. The effect of synthesis conditions, such as irradiation time and gas environment, was investigated. The structure and formation mechanism of the carbide phases were explored. As-synthesized nanomaterials exhibited catalytic activity for hydrous hydrazine (N2H4·H2O) decomposition at 30-70 °C. It was shown that the catalyst activity significantly increases if microwave irradiation is applied during the decomposition process. Such conditions permit complete conversion of hydrazine to ammonia and nitrogen within minutes. This effect can be attributed to the unique nanostructure of the catalysts that includes microwave absorbing carbon and active carbide constituents.

  19. Facile One-Step Synthesis of Hybrid Graphitic Carbon Nitride and Carbon Composites as High-Performance Catalysts for CO2 Photocatalytic Conversion.

    Science.gov (United States)

    Wang, Yangang; Bai, Xia; Qin, Hengfei; Wang, Fei; Li, Yaguang; Li, Xi; Kang, Shifei; Zuo, Yuanhui; Cui, Lifeng

    2016-07-13

    Utilizing and reducing carbon dioxide is a key target in the fight against global warming. The photocatalytic performance of bulk graphitic carbon nitride (g-C3N4) is usually limited by its low surface area and rapid charge carrier recombination. To develop g-C3N4 more suitable for photocatalysis, researchers have to enlarge its surface area and accelerate the charge carrier separation. In this work, novel hybrid graphitic carbon nitride and carbon (H-g-C3N4/C) composites with various carbon contents have been developed for the first time by a facile one-step pyrolysis method using melamine and natural soybean oil as precursors. The effect of carbon content on the structure of H-g-C3N4/C composites and the catalytic activity for the photoreduction of CO2 with H2O were investigated. The results indicated that the introduction of carbon component can effectively improve the textural properties and electronic conductivity of the composites, which exhibited imporved photocatalytic activity for the reduction of CO2 with H2O in comparison with bulk g-C3N4. The highest CO and CH4 yield of 22.60 μmol/g-cat. and 12.5 μmol/g-cat., respectively, were acquired on the H-g-C3N4/C-6 catalyst with the carbon content of 3.77 wt % under 9 h simulated solar irradiation, which were more than twice as high as that of bulk g-C3N4. The remarkably increased photocatalytic performance arises from the synergistic effect of hybrid carbon and g-C3N4. PMID:27112547

  20. Facile One-Step Synthesis of Hybrid Graphitic Carbon Nitride and Carbon Composites as High-Performance Catalysts for CO2 Photocatalytic Conversion.

    Science.gov (United States)

    Wang, Yangang; Bai, Xia; Qin, Hengfei; Wang, Fei; Li, Yaguang; Li, Xi; Kang, Shifei; Zuo, Yuanhui; Cui, Lifeng

    2016-07-13

    Utilizing and reducing carbon dioxide is a key target in the fight against global warming. The photocatalytic performance of bulk graphitic carbon nitride (g-C3N4) is usually limited by its low surface area and rapid charge carrier recombination. To develop g-C3N4 more suitable for photocatalysis, researchers have to enlarge its surface area and accelerate the charge carrier separation. In this work, novel hybrid graphitic carbon nitride and carbon (H-g-C3N4/C) composites with various carbon contents have been developed for the first time by a facile one-step pyrolysis method using melamine and natural soybean oil as precursors. The effect of carbon content on the structure of H-g-C3N4/C composites and the catalytic activity for the photoreduction of CO2 with H2O were investigated. The results indicated that the introduction of carbon component can effectively improve the textural properties and electronic conductivity of the composites, which exhibited imporved photocatalytic activity for the reduction of CO2 with H2O in comparison with bulk g-C3N4. The highest CO and CH4 yield of 22.60 μmol/g-cat. and 12.5 μmol/g-cat., respectively, were acquired on the H-g-C3N4/C-6 catalyst with the carbon content of 3.77 wt % under 9 h simulated solar irradiation, which were more than twice as high as that of bulk g-C3N4. The remarkably increased photocatalytic performance arises from the synergistic effect of hybrid carbon and g-C3N4.

  1. The synergistic effect in the Fe-Co bimetallic catalyst system for the growth of carbon nanotube forests

    Energy Technology Data Exchange (ETDEWEB)

    Hardeman, D.; Esconjauregui, S., E-mail: cse28@cam.ac.uk; Cartwright, R.; D' Arsié, L.; Robertson, J. [Department of Engineering, University of Cambridge, Cambridge CB3 0FA (United Kingdom); Bhardwaj, S.; Cepek, C. [Istituto Officina dei Materiali-CNR, Laboratorio TASC, Trieste I-34149 (Italy); Oakes, D.; Clark, J. [Johnson Matthey Technology Centre, Sonning Common RG4 9NH (United Kingdom); Ducati, C. [Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS (United Kingdom)

    2015-01-28

    We report the growth of multi-walled carbon nanotube forests employing an active-active bimetallic Fe-Co catalyst. Using this catalyst system, we observe a synergistic effect by which—in comparison to pure Fe or Co—the height of the forests increases significantly. The homogeneity in the as-grown nanotubes is also improved. By both energy dispersive spectroscopy and in-situ x-ray photoelectron spectroscopy, we show that the catalyst particles consist of Fe and Co, and this dramatically increases the growth rate of the tubes. Bimetallic catalysts are thus potentially useful for synthesising nanotube forests more efficiently.

  2. Enantioselective Alternating Copolymerization of Propylene with Carbon Monoxide Using Cationic Palladium-Chiral Diphosphine Catalyst

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Enantioselective alternating copolymerization of carbon monoxide with propylene was carried out using palladium catalyst modified by 1,4-3,6-dianhydro-2,5-dideoxy-2,5-bis (diphenylphosphino)-L-iditol (DDPPI). The chiral diphosphine was proved to be effective at enantioselective copolymerization. Optical rotation, elemental analysis, 1H, 13C-NMR and IR spectra showed that the copolymer was optically active, isotactic, alternating poly(1,4-ketone) structure.

  3. Manganese Detection with a Metal Catalyst Free Carbon Nanotube Electrode: Anodic versus Cathodic Stripping Voltammetry

    OpenAIRE

    Yue, Wei; Bange, Adam; Riehl, Bill L.; Riehl, Bonnie D.; Johnson, Jay M.; Papautsky, Ian; Heineman, William R.

    2012-01-01

    Anodic stripping voltammetry (ASV) and cathodic stripping voltammetry (CSV) were used to determine Mn concentration using metal catalyst free carbon nanotube (MCFCNT) electrodes and square wave stripping voltammetry (SWSV). The MCFCNTs are synthesized using a Carbo Thermal Carbide Conversion method which results in a material that does not contain residual transition metals. Detection limits of 120 nM and 93 nM were achieved for ASV and CSV, respectively, with a deposition time of 60 s. CSV w...

  4. Kinetics of wet oxidation of phenol over an Fe/activated carbon catalyst

    NARCIS (Netherlands)

    Quintanilla, A.; Casas, J.A.; Rodriquez, J.J.; Kreutzer, M.T.; Kapteijn, F.; Moulijn, J.A.

    2007-01-01

    Wet oxidation of phenol over an Fe/activated carbon catalyst has been studied in a trickle-bed reactor in the following operational window: inlet C phenol=0.5 and 1 g/L, T=100-127 ºC, PT=3-8 atm, W=0-4.8 g, QL=0.125-2 mL/min and QO2=91.6 NmL/min. The experiments were carried out in the absence of ma

  5. Direct synthesis of dimethyl carbonate and propylene glycol using potassium bicarbonate as catalyst in supercritical CO2

    OpenAIRE

    Wen Yicun; Zhang Rui; Cang Yu; Zhang Jianchao; Liu Lixiao; Guo Xuhong; Fan Bin

    2015-01-01

    The improved one-pot synthesis of dimethyl carbonate and propylene glycol from propylene oxide, supercritical carbon dioxide, and methanol with potassium bicarbonate as the catalyst has been reported in this paper. As far as we know, it is the first time to use potassium bicarbonate only as the catalyst in the production process which is simple and cheap. Satisfactory conversion rate of propylene oxide and yield of the products could be achieved at the optimized conditions with quite a small ...

  6. Growth Mechanism of Single-Walled Carbon Nanotubes on Iron–Copper Catalyst and Chirality Studies by Electron Diffraction

    DEFF Research Database (Denmark)

    He, Maoshuai; Liu, Bilu; Chernov, Alexander I.;

    2012-01-01

    Chiralities of single-walled carbon nanotubes grown on an atomic layer deposition prepared bimetallic FeCu/MgO catalyst were evaluated quantitatively using nanobeam electron diffraction. The results reveal that the growth yields nearly 90% semiconducting tubes, 45% of which are of the (6,5) type...... by impregnation, showing similar catalytic performance as the atomic layer deposition-prepared catalyst, yielding single-walled carbon nanotubes with a similar narrow chirality distribution....

  7. Carbon : nickel nanocomposite templates - predefined stable catalysts for diameter-controlled growth of single-walled carbon nanotubes

    Science.gov (United States)

    Melkhanova, Svetlana; Haluska, Miro; Hübner, René; Kunze, Tim; Keller, Adrian; Abrasonis, Gintautas; Gemming, Sibylle; Krause, Matthias

    2016-08-01

    Carbon : nickel (C : Ni) nanocomposite templates (NCTs) were used as catalyst precursors for diameter-controlled growth of single-walled carbon nanotubes (SWCNTs) by chemical vapor deposition (CVD). Two NCT types of 2 nm thickness were prepared by ion beam co-sputtering without (type I) or with assisting Ar+ ion irradiation (type II). NCT type I comprised Ni-rich nanoparticles (NPs) with defined diameter in an amorphous carbon matrix, while NCT type II was a homogenous C : Ni film. Based on the Raman spectra of more than 600 individual SWCNTs, the diameter distribution obtained from both types of NCT was determined. SWCNTs with a selective, monomodal diameter distribution are obtained from NCT type I. About 50% of the SWCNTs have a diameter of (1.36 +/- 0.10) nm. In contrast to NCT type I, SWCNTs with a non-selective, relatively homogeneous diameter distribution from 0.80 to 1.40 nm covering 88% of all SWCNTs are obtained from NCT type II. From both catalyst templates predominantly separated as-grown SWCNTs are obtained. They are free of solvents or surfactants, exhibit a low degree of bundling and contain negligible amounts of MWCNTs. The study demonstrates the advantage of predefined catalysts for diameter-controlled SWCNT synthesis in comparison to in situ formed catalysts.Carbon : nickel (C : Ni) nanocomposite templates (NCTs) were used as catalyst precursors for diameter-controlled growth of single-walled carbon nanotubes (SWCNTs) by chemical vapor deposition (CVD). Two NCT types of 2 nm thickness were prepared by ion beam co-sputtering without (type I) or with assisting Ar+ ion irradiation (type II). NCT type I comprised Ni-rich nanoparticles (NPs) with defined diameter in an amorphous carbon matrix, while NCT type II was a homogenous C : Ni film. Based on the Raman spectra of more than 600 individual SWCNTs, the diameter distribution obtained from both types of NCT was determined. SWCNTs with a selective, monomodal diameter distribution are obtained from NCT

  8. Characterization and Design of Zeolite Catalysts Solid Acidity, Shape Selectivity and Loading Properties

    CERN Document Server

    Niwa, Miki; Okumura, Kazu

    2010-01-01

    Zeolites are microporous, aluminosilicate minerals commonly used as commercial adsorbents. Zeolite-based catalysts are used by industrial chemical companies in the interconversion of hydrocarbons and the alkylation of aromatic compounds. The current book deals with the characterization of specific properties of Zeolites and calculations for the design of catalysts. Measurements and utilization of solid acidity, shape selectivity, and loading properties, that are three prominent properties of a Zeolite catalyst, are treated in detail. These features concern chemical vapor deposition of silica, shape selectivity, loading properties, solid activity, Brønsted or Lewis character, ammonia temperature programmed desorption, control of the pore-opening size by chemical vapor deposition of silica and XAFS analysis of metals being highly dispersed inside and outside a framework.

  9. Oxygen and nitrogen-doped metal-free carbon catalysts for hydrochlorination of acetylene☆

    Institute of Scientific and Technical Information of China (English)

    Tongtong Zhang; Jia Zhao; Jiangtao Xu; Jinhui Xu; Xiaoxia Di; Xiaonian Li

    2016-01-01

    Activated carbon was tested as metal-free catalyst for hydrochlorination of acetylene in order to circumvent the problem of environment pollution caused by mercury and high cost by noble metals. Oxygen-doped and nitrogen-doped activated carbons were prepared and characterized by XPS, TPD and N2 physisorption methods. The influences of the surface functional groups on the catalytic performance were discussed base on these results. Among al the samples tested, a nitrogen-doped sample, AC-n-U500, exhibited the best performance, the acety-lene conversion being 92%and vinyl chloride selectivity above 99%at 240 °C and C2H2 hourly space velocity 30 h−1. Moreover, the AC-n-U500 catalyst exhibited a stable performance during a 200 h test with a conversion of acetylene higher than 76%at 210 °C at a C2H2 hourly space velocity 50 h−1. In contrary, oxygen-doped catalyst had lower catalytic activities. A linear relationship between the amount of pyrrolic-N and quaternary-N species and the catalytic activity was observed, indicating that these nitrogen-doped species might be the active sites and the key in tuning the catalytic performance. It is also found that the introduction of nitrogen species into the sample could significantly increase the adsorption amount of acetylene. The deactivation of nitrogen-doped activated carbon might be caused by the decrease of the accessibility to or the total amount of active sites.

  10. Strength and microplasticity of biocarbons prepared by carbonization in the presence of a catalyst

    Science.gov (United States)

    Shpeizman, V. V.; Orlova, T. S.; Smirnov, B. I.; Gutierrez-Pardo, A.; Ramirez-Rico, J.

    2016-04-01

    The microdeformation has been investigated under uniaxial compression of beech-derived biocarbons partially graphitized during carbonization in the presence of a Ni- or Fe-containing catalyst. The strength and ultimate fracture strain have been determined at different temperatures of carbonization of the samples in the absence or in the presence of a catalyst. It has been shown using high-precision interferometry that the deformation of biocarbon samples under uniaxial loading occurs through jumps (in magnitude and rate of deformation) with axial displacements in the nanometer and micrometer ranges. The use of a catalyst leads to a decrease in the size of nanometer-scale jumps and in the number of micrometer-scale jumps. The standard deviations of the strain rate on loading steps from the smooth average dependence of the strain rate on the displacement have been calculated for micrometer-scale jumps. A similar characteristic for nanometer- scale jumps has been determined from the distortion of the shape of beats in the primary interferogram. It has been shown that the variation in the standard deviation of the strain rate with a change in the carbonization temperature is similar to the corresponding dependence of the ultimate fracture strain.

  11. NiO/CeO2-ZnO nano-catalysts for direct synthesis of dimethyl carbonate from methanol and carbon dioxide.

    Science.gov (United States)

    Kang, Ki Hyuk; Lee, Chang Hoon; Kim, Dong Baek; Jang, Boknam; Song, In Kyu

    2014-11-01

    XNiO/CeO2(0.7)-ZnO(0.3) (X = 0, 1, 5, 10, and 15) nano-catalysts were prepared by a wet impregnation method with a variation of NiO content (X, wt%). The prepared catalysts were then applied to the direct synthesis of dimethyl carbonate from methanol and carbon dioxide. Successful formation of XNiO/CeO2(0.7)-ZnO(0.3) nano-catalysts was confirmed by XRD and ICP-AES analyses. Acidity and basicity of XNiO/CeO2-ZnO were measured by NH3-TPD (temperature-programmed desorption) and CO2-TPD experiments, respectively, with an aim of elucidating the effect of acidity and basicity of the catalysts on the catalytic performance in the reaction. It was revealed that the catalytic activity of XNiO/CeO2(0.7)-ZnO(0.3) was closely related to both acidity and basicity of the catalysts. The amount of dimethyl carbonate produced over XNiO/CeO2(0.7)-ZnO(0.3) increased with increasing acidity and basicity of the catalysts. Thus, both acidity and basicity of the catalysts played important roles in determining the catalytic performance in the direct synthesis of dimethyl carbonate from methanol and carbon dioxide. PMID:25958586

  12. Effect of solvent on Se-modified ruthenium/carbon catalyst for oxygen reduction

    OpenAIRE

    Chuanxiang Zhang; Haijun Tao; Yuming Dai; Xiancong He; Kejie Zhang

    2014-01-01

    Se-modified ruthenium supporting on carbon (Sex–Ru/C) electrocatalyst was prepared by solvothermal one-step synthesis method. The reaction mechanism was revealed after discussing impact of different solvents (i-propanol and EG) in solvotermal reaction. The result showed that the grain size of Se-modified ruthenium electrocatalyst was as small as 1 to 3 nm and highly dispersed on carbon surface. X-ray photoelectron spectroscopy (XPS) presented that selenium mainly existed in the catalyst in th...

  13. Interaction of carbon monoxide and oxygen at the surface of inverse titania/Au model catalyst

    Science.gov (United States)

    Magkoev, Tamerlan T.

    2007-07-01

    Interaction of carbon monoxide and oxygen on the surface of titania/Au(1 1 1) inverse model catalyst held at 200 K has been studied by reflection absorption infrared spectroscopy. It was found that CO adsorbs on the oxide/Au perimeter interface, whereas no or very weak adsorption was observed on Au(1 1 1) or titania surface, respectively. Exposing of such species to oxygen results in their decay possibly due to carbon dioxide formation. Efficiency of this effect is higher at lower CO initial concentration which points at the importance of free surface sites for the reaction process.

  14. Effect of solvent on Se-modified ruthenium/carbon catalyst for oxygen reduction

    Institute of Scientific and Technical Information of China (English)

    Chuanxiang Zhang; Haijun Tao; Yuming Dai; Xiancong He; Kejie Zhang

    2014-01-01

    Se-modified ruthenium supporting on carbon (Sex–Ru/C) electrocatalyst was prepared by solvothermal one-step synthesis method. The reaction mechanism was revealed after discussing impact of different solvents (i-propanol and EG) in solvotermal reaction. The result showed that the grain size of Se-modified ruthenium electrocatalyst was as small as 1 to 3 nm and highly dispersed on carbon surface. X-ray photoelectron spectroscopy (XPS) presented that selenium mainly existed in the catalyst in the form of elemental selenium and selenium oxides when the solvent was EG and i-propanol, respectively. The oxygen reduction reaction (ORR) performance was improved by appearance of selenium oxides.

  15. Porous polymers bearing functional quaternary ammonium salts as efficient solid catalysts for the fixation of CO2 into cyclic carbonates

    Science.gov (United States)

    Cai, Sheng; Zhu, Dongliang; Zou, Yan; Zhao, Jing

    2016-07-01

    A series of porous polymers bearing functional quaternary ammonium salts were solvothermally synthesized through the free radical copolymerization of divinylbenzene (DVB) and functionalized quaternary ammonium salts. The obtained polymers feature highly cross-linked matrices, large surface areas, and abundant halogen anions. These polymers were evaluated as heterogeneous catalysts for the synthesis of cyclic carbonates from epoxides and CO2 in the absence of co-catalysts and solvents. The results revealed that the synergistic effect between the functional hydroxyl groups and the halide anion Br- afforded excellent catalytic activity to cyclic carbonates. In addition, the catalyst can be easily recovered and reused for at least five cycles without significant loss in activity.

  16. Fe-Ti-O based catalyst for large-chiral-angle single-walled carbon nanotube growth

    DEFF Research Database (Denmark)

    He, Maoshuai; Zhang, Lili; Jiang, Hua;

    2016-01-01

    Catalyst selection is very crucial for controlled growth of single-walled carbon nanotubes (SWNTs). Here we introduce a well-designed Fe-Ti-O solid solution for SWNT growth with a high preference to large chiral angles. The Fe-Ti-O catalyst was prepared by combining Ti layer deposition onto premade...... Fe nanoparticles with subsequent high-temperature air calcination, which favours the formation of a homogeneous Fe-Ti-O solid solution. Using CO as the carbon feedstock, chemical vapour deposition growth of SWNTs at 800 °C was demonstrated on the Fe-Ti-O catalyst. Nanobeam electron diffraction...

  17. Synthesis of glycerol Carbonate from glycerol and urea using zinc-containing solid catalysts: A homogeneous reaction

    OpenAIRE

    Fujita, Shin-ichiro; Yamanishi, Yuki; Arai, Masahiko

    2013-01-01

    Zinc-containing solid catalysts (zinc oxide, smectite, hydrotalcite) and several inorganic zinc salts were used to produce glycerol carbonate from glycerol and urea under solvent-free conditions at 130℃ and at a reduced pressure of 3 kPa. The leaching of Zn species was observed to occur for the solid catalysts and the carbonate yield was shown to be correlated with the amount of zinc species dissolved into the liquid phase with a single relationship in common for all the catalysts employed. T...

  18. The Electrochemical Performance and Durability of Carbon Supported Pt Catalyst in Contact with Aqueous and Polymeric Proton Conductors

    DEFF Research Database (Denmark)

    Andersen, Shuang Ma; Skou, Eivind Morten

    2014-01-01

    supported platinum catalyst in four different electrode structures: catalyst powder (CP), catalyst ionomer electrode (CIE), half membrane electrode assembly (HMEA) and full membrane electrode assembly (FMEA) in both ex-situ and in-situ experiments under a simulated start/stop cycle. We found......Significant differences in catalyst performance and durability are often observed between the use of a liquid electrolyte (e.g. sulfuric acid), and a solid polymer electrolyte (e.g. Nafion®). To understand this phenomenon, we studied the electrochemical behavior of a commercially available carbon...... that the catalyst performance and stability are very much influenced by the presence of the Nafion ionomers. The proton conducting phase provided by the ionomer and the self-assembled electrode structure render the catalysts a higher utilization and better stability. This is probably due to an enhanced dispersion...

  19. Low-temperature catalyst activator: mechanism of dense carbon nanotube forest growth studied using synchrotron radiation

    Directory of Open Access Journals (Sweden)

    Akito Takashima

    2014-07-01

    Full Text Available The mechanism of the one-order-of-magnitude increase in the density of vertically aligned carbon nanotubes (CNTs achieved by a recently developed thermal chemical vapor deposition process was studied using synchrotron radiation spectroscopic techniques. In the developed process, a Ti film is used as the underlayer for an Fe catalyst film. A characteristic point of this process is that C2H2 feeding for the catalyst starts at a low temperature of 450°C, whereas conventional feeding temperatures are ∼800°C. Photoemission spectroscopy using soft and hard X-rays revealed that the Ti underlayer reduced the initially oxidized Fe layer at 450°C. A photoemission intensity analysis also suggested that the oxidized Ti layer at 450°C behaved as a support for nanoparticle formation of the reduced Fe, which is required for dense CNT growth. In fact, a CNT growth experiment, where the catalyst chemical state was monitored in situ by X-ray absorption spectroscopy, showed that the reduced Fe yielded a CNT forest at 450°C. Contrarily, an Fe layer without the Ti underlayer did not yield such a CNT forest at 450°C. Photoemission electron microscopy showed that catalyst annealing at the conventional feeding temperature of 800°C caused excess catalyst agglomeration, which should lead to sparse CNTs. In conclusion, in the developed growth process, the low-temperature catalyst activation by the Ti underlayer before the excess Fe agglomeration realised the CNT densification.

  20. Fabrication of functional hollow carbon spheres with large hollow interior as active colloidal catalysts

    Institute of Scientific and Technical Information of China (English)

    Qiang Sun; Guanghui Wang; Wencui Li; Xiangqian Zhang; Anhui Lu

    2012-01-01

    In this study,we have established a facile method to synthesize functional hollow carbon spheres with large hollow interior,which can act as active colloidal catalysts.The method includes the following steps:first,hollow polymer spheres with large hollow interior were prepared using sodium oleate as the hollow core generator,and 2,4-dihydroxybenzoic acid and hexamethylene tetramine (HMT) as the polymer precursors under hydrothermal conditions; Fe3+ or Ag+ cations were then introduced into the as-prepared hollow polymer spheres through the carboxyl groups; finally,the hollow polymer spheres can be pseudomorphically converted to hollow carbon spheres during pyrolysis process,meanwhile iron or silver nanoparticles can also be formed in the carbon shell simultaneously.The structures of the obtained functional hollow carbon spheres were characterized by TEM,XRD,and TG.As an example,Ag-doped hollow carbon spheres were used as colloid catalysts which showed high catalytic activity in 4-nitrophenol reduction reaction.

  1. Fabrication and Properties of Carbon Fibers

    Directory of Open Access Journals (Sweden)

    Xiaosong Huang

    2009-12-01

    Full Text Available This paper reviews the research and development activities conducted over the past few decades on carbon fibers. The two most important precursors in the carbon fiber industry are polyacrylonitrile (PAN and mesophase pitch (MP. The structure and composition of the precursor affect the properties of the resultant carbon fibers significantly. Although the essential processes for carbon fiber production are similar, different precursors require different processing conditions in order to achieve improved performance. The research efforts on process optimization are discussed in this review. The review also attempts to cover the research on other precursor materials developed mainly for the purpose of cost reduction.

  2. STUDY ON THE MECHANICAL PROPERTIES OF SOLID CATALYSTS

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    IntroductionMixed oxides and oxide-supported metalcatalysts are widely used in the petroleum andchemical industries. Besides aGtivity and selectivity, asuccessful solid catalyst should have good physicalproperties, among which mechanical strength is one ofthe key parameters for the reliable and efficientperformance of a fi'xed bed converterlll. Duringtransportation as well as in operation, the catalystssuffer from mechanical stress, which can besufficiently high to cause fracture of the particle. Theformati...

  3. THE FABRICATION OF CARBON AEROGELS BY GELATION IN ISOPROPANOL WITH BASIC CATALYST

    Institute of Scientific and Technical Information of China (English)

    WU Dingcai; ZHANG Shuting; FU Ruowen

    2003-01-01

    A new method for the fabrication of carbon aerogels is reported in this paper. Resorcinol and furfural were gelated in isopropanol with basic catalysts and then dried directly under isopropanol supercritical condition, followed by carbonization under nitrogen atmosphere. The bulk densities of carbon aerogels obtained are in the range of 0. 21g/cm3~0. 27g/cm3 and the sizes of the interconnected carbon nano-particles are in the range of 20nm~30nm. All of the aerogel samples exhibit high BET surface areas in the range of 730m2/g~900m2/g. The bulk density, micro-porevolume, meso-pore volume and meso-pore diameter can be controlled by gelation conditions such as R/I ratio and R/C ratio.

  4. sup 1 H NMR studies of hydrogen and carbon monoxide chemisorption on the EUROPt-1 catalyst

    CERN Document Server

    Bouyssy, P X

    2001-01-01

    possible carbon monoxide-induced reorganisation of the surface sites available for hydrogen, following a carbon monoxide precoverage above a critical level. It also shows that carbon monoxide blocks hydrogen adsorption but not in the manner expected. No desorption of carbon monoxide was observed with gas phase infrared experiments even at hydrogen coverages approaching saturation. Secondly, to further the understanding of the dynamics of adsorbed hydrogen exchanging between the strongly bound and the weakly bound sites, proton relaxation NMR experiments were undertaken. T sub 1 and T sub 1 subrho measurements were carried out as a function of hydrogen coverage at room temperature and as a function of temperature at fixed hydrogen coverage. These experiments proved to be experimentally challenging and the data obtained do not show a clear enough trend to reach a significant conclusion as was firstly expected. A specially designed sup 1 H NMR probe, capable of holding a large quantity of catalyst sample for in ...

  5. An investigation into carbon nanostructured materials as catalyst support in proton exchange membrane fuel cells

    DEFF Research Database (Denmark)

    Veltzé, Sune

    Polymer electrolyte fuel cells (PEFCs) are among the key research areas concerning clean cost-effective energy. Carbon nano fibres (CNF), single walled carbon nano tubes (SWCNT), multi walled carbon nano tubes (MWCNT) and other related materials are among the possible successors to standard carbon...... used in the characterisation of different platinised CNF and MWCNT, to evaluate their performance as a fuel cell catalyst for the hydrogen oxidation reaction (HOR) and oxygen reduction reaction (ORR) are made. The need for using an dispersion agent was inferred as the electrochemical RDE and RRDE did...... not adhere to the theoretical conditions. The use of dispersion agents induced however a necessity to re-evaluate the thin-film method so that the ancillary agents effect of the kinetics could be neglected. Furthermore, different characterisation methods are used for evaluating the effect of the corrosive...

  6. Preparation and Characterization of Carbon Nanotubes-Coated Cordierite for Catalyst Supports

    Institute of Scientific and Technical Information of China (English)

    Jianmei Wang; Rong Wang; Xiujin Yu; Jianxin Lin; Feng Xie; Kemei Wei

    2006-01-01

    The carbon nanotubes-coated cordierite (CNTs-cordierite) was fabricated by pyrolysis of ethine on cordierite with iron catalyst, which was penetrated into the cordierite substrate by vacuum impregnation. The cordierite substrate, carbon naontubes, and CNTs-cordierite were characterized by SEM, TEM/HREM, BET, and TGA. The results show that the carbon nanotubes were distributed uniformly on the surface of cordierite. A significant increase in BET surface area and pore volume was observed, and a suitable pore-size distribution was obtained. On the CNTs-cordierite, carbon nanotubes penetrated into the cordierite substrate, which led to a remarkable stability of the CNTs against ultrasound maltreatment. Growth time is an important factor for thermostability and texture of the sample. The mass increased but the purity decreased with the growth time, which caused the exothermic peak shift to low temperature, and the corresponding full width half maximum (FWHM) of the peak in DTG increased.

  7. Immobilised carbon nanotubes as carrier for Co-Fischer-Tropsch synthesis catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Thiessen, J.; Rose, A.; Kiendl, I.; Jess, A. [Bayreuth Univ. (Germany). Dept. of Chemical Engineering; Curulla-Ferre, D. [Total S.A., Gas and Power, Paris La Defense (France)

    2011-07-01

    A possibility to immobilise carbon nanotubes (CNT) to make them applicable in a technical scale fixed bed reactor is studied. The approach to fabricate millimetre scale composites containing CNT presented in this work is to confine the nano-carbon in macro porous ceramic particles. Thus CNT were grown on the inner surface of silica and alumina pellets and spheres, respectively. Cobalt nano particles were successfully deposited on the carbon surface inside the two types of ceramic carriers and the systems were tested in Fischer - Tropsch synthesis (FTS). The cobalt mass related activity of these novel catalysts is similar to a conventional system. The selectivities of the Co/CNT/ceramic composites were compared with non supported CNT and carbon nanofibres (CNF). (orig.)

  8. Preparation-Properties Relation of Mn-Cu Hopcalite Catalyst

    Directory of Open Access Journals (Sweden)

    Ardita Mele

    2012-01-01

    Full Text Available Problem statement: The Mn-Cu hopcalite catalyst was used for the conversion of CO to CO2 at low temperatures. It was the catalyst of choice in the gas masks for respiratory protection in mines, aircrafts, military, spatial laboratories. Approach: The efficiency of hopcalite catalyst depends on its surface parameters. Its surface characteristics can be influenced from the chosen way of the MnO2 and CuO precipitation and from the pressure of pelletizing. Results: The hopcalite samples has been prepared by precipitation of MnO2 and by adding CuSO4 further in the solution the adsorption of Cu2+ ions on MnO2 particles surface is achieved. After acidification of the solution up to pH = 3 the copper is precipitated in form of Cu (OH2CuCO3 by adding NaHCO3. Precipitate was washed, dried, pressed, crushed, sieved (1-2 mm and calcined at 180°C for 3 h. MnO2 and hopcalite samples were characterized by XRD. The activity was evaluated by determination of its protection time and it was 610 min, better than activity of a commercial catalyst. Specific surface area, pore volume and density were measured by nitrogen adsorption and mercury intrusion porosimetry. The X-Ray diffractograms shows that the only crystallinity of hopcalite comes from MnO2, which is present mainly in amorphous form. By increasing the pressure in the pelletizing step, a significant decrease in the specific surface area (247.64-147.77 m2 g-1 and in the total pore volume (446-278 mm3 g-1 is observed in the hopcalite samples. Conclusion: The obtained hopcalite catalyst by the two step precipitation method shows high catalytic activity. The increasing pressure increases the strength and reduces the specific surface area and pore volume. A pressure of 500 kg cm-2 is recommended for the hopcalite production procedure.

  9. Heteropoly Acid/Nitrogen Functionalized Onion-like Carbon Hybrid Catalyst for Ester Hydrolysis Reactions.

    Science.gov (United States)

    Liu, Wei; Qi, Wei; Guo, Xiaoling; Su, Dangsheng

    2016-02-18

    A novel heteropoly acid (HPA)/nitrogen functionalized onion-like carbon (NOLC) hybrid catalyst was synthesized through supramolecular (electrostatic and hydrogen bond) interactions between the two components. The chemical structure and acid strength of the HPA/NOLC hybrid have been fully characterized by thermogravimetric analysis, IR spectroscopy, X-ray photoelectron spectroscopy, NH3 temperature-programmed desorption and acid-base titration measurements. The proposed method for the fabrication of the HPA/NOLC hybrid catalyst is a universal strategy for different types of HPAs to meet various requirements of acidic or redox catalysis. The hydrophobic environment of NOLC effectively prevents the deactivation of HPA in an aqueous system, and the combination of uniformly dispersed HPA clusters and the synergistic effect between NOLC and HPA significantly promotes its activity in ester hydrolysis reactions, which is higher than that of bare PWA as homogeneous catalyst. The kinetics of the hydrolysis reactions indicate that the aggregation status of the catalyst particles has great influence on the apparent activity. PMID:26606266

  10. Molecular dynamics study of the catalyst particle size dependence on carbon nanotube growth

    Science.gov (United States)

    Ding, Feng; Rosén, Arne; Bolton, Kim

    2004-08-01

    The molecular dynamics method, based on an empirical potential energy surface, was used to study the effect of catalyst particle size on the growth mechanism and structure of single-walled carbon nanotubes (SWNTs). The temperature for nanotube nucleation (800-1100 K), which occurs on the surface of the cluster, is similar to that used in catalyst chemical vapor deposition experiments, and the growth mechanism, which is described within the vapor-liquid-solid model, is the same for all cluster sizes studied here (iron clusters containing between 10 and 200 atoms were simulated). Large catalyst particles, which contain at least 20 iron atoms, nucleate SWNTs that have a far better tubular structure than SWNTs nucleated from smaller clusters. In addition, the SWNTs that grow from the larger clusters have diameters that are similar to the cluster diameter, whereas the smaller clusters, which have diameters less than 0.5 nm, nucleate nanotubes that are ≈0.6-0.7 nm in diameter. This is in agreement with the experimental observations that SWNT diameters are similar to the catalyst particle diameter, and that the narrowest free-standing SWNT is 0.6-0.7 nm.

  11. Activation of model nickel catalysts for hydrogenation of carbon dioxide to methane

    Energy Technology Data Exchange (ETDEWEB)

    Barcicki, J.; Grzegorczyk, W.; Borowiecki, T.; Nazimek, D.; Denis, A.

    1977-09-01

    In studies related to steam reforming of hydrocarbons and to hydrogenation, the reaction of hydrogen with carbon dioxide in a 5:1 ratio at 400/sup 0/C for ten hr in a Carberry differential reactor over reduced nickel catalyst containing 0-10% of cobalt, copper, or iron metal, or of an oxide of potassium, zinc, barium, calcium, magnesium, chromium, or aluminum gave the best results over catalysts containing one of the last three oxides. The results included respective activity losses of 24.2, 20.4, and 7.24%; respective initial selectivities of 98.3, 98.5, and 97.6; respective final selectivities of 93.6, 95.9, and 96.6; and much higher activities, which increased with increasing promoter content; alumina gave the highest activity. Catalyst preparation and the role of the most effective promoters in increasing the active surface via changes in crystallite structure, and in improving catalyst thermal stability are discussed. Graphs, tables, and 22 references.

  12. Transition metal-modified polyoxometalates supported on carbon as catalyst in 2-(methylthio)-benzothiazole sulfoxidation

    Indian Academy of Sciences (India)

    Romina A Frenzel; Gustavo P Romanelli; Mirta N Blanco; Luis R Piz

    2015-01-01

    Polyoxometalates with lacunary Keggin structure modified with transition metal ions [PW11O39M(H2O)]5−, where M = Ni2+, Co2+, Cu2+ or Zn2+, were synthesized and supported on activated carbon to obtain the PW11MC catalysts. Using FT-IR and DTA-TGA it was concluded that the [PW11O39M(H2O)]5− species are interacting with the functional groups of the support, and that thermal treatment leads to the loss of the coordinatively bonded water molecules without any noticeable anion degradation. The activity and selectivity of the catalysts in the sulfoxidation reaction of 2-(methylthio)-benzothiazole, an emerging environmental pollutant, were evaluated. The reaction was carried out in acetonitrile as solvent using H2O2 35% p/v as a clean oxidant. The conversion values decreased in the following order: PW11NiC > PW11CuC > PW11CoC > PW11ZnC, with selectivity to sulfoxide higher than 69%. The catalyst could be reused without appreciable loss of the catalytic activity at least three times. The materials were found to be efficient and recyclable catalysts for 2-(methylthio)-benzothiazole sulfoxidation in order to obtain a more biodegradable product than the corresponding substrate.

  13. PREPARATION OF MULTI-WALLED CARBON NANOTUBES USING NiO CATALYST SYNTHESIZED BY HYDROTHERMAL METHOD

    Institute of Scientific and Technical Information of China (English)

    Y.J. Zhu; Y.L. Chen; X.M. Xue; Y.M. Chen; C.Y. Wu; T.C. Kuang; S.H. Li; H. Y. Zhang

    2003-01-01

    The Ni(OH)2/SiO2 binary colloid was prepared using Ni(NO3)2.6H2O and (C2H5 O)4SiO4 as starting materials and was used to form NiO/SiO2 composite powder by hydrothermal method and desiccant method in open air respectively. Multiwalled carbon nanotubes (MWCNTs) were synthesized respectively by chemical vapor deposition using the NiO/SiO2 catalyst prepared by different methods. The phase and morphology of the catalysts and the morphology, output yield and purity of MWCNTs were compared by XRD, TEM and SEM. The results show that the catalyst powder prepared by hydrothermal method, compared with that by desiccant method, is smaller, better dispersion and has stronger catalytic activity. Pure MWCNTs with smaller tube diameter and narrow range could be obtained at a high yield using that NiO/SiO.2 powder prepared by hydrothermal method as catalyst.

  14. Methane dry reforming catalysts for the production of hydrogen and carbon monoxide

    International Nuclear Information System (INIS)

    The reaction of carbon dioxide reforming of methane (dry reforming) is a very attractive way to convert low-cost reactants in synthesis gas (CO + H2).Moreover, the reaction also has very important environmental effects because both methane and carbon dioxide are greenhouse gases, and may become valuable raw materials. One of the advantages of the dry reforming compared with the conventional steam reforming is the low H2:CO relationship in the product, which is preferred for the synthesis of oxoalcohols and oxygenated compounds. Although noble metals based catalysts have been proved to be less sensitive to coke, the high cost and restricted availability limit their use in this process.From an industrial standpoint, it is more desirable to develop nickel-based catalysts, which are resistant to carbon deposition and exhibit stable operation for extended periods of time.In this work nickel-alumina catalysts, pure or promoted with rhodium or ruthenium, were prepared using different techniques, employing aluminum and nickel alkoxides, and characterized and selected according to their catalytic activity and coking resistance.These catalysts are to be used in an inert ceramic membrane reactor.The nickel precursor is a nickel alkoxide incorporated to the matrix precursor of alumina, which at the same time is an aluminum alkoxide.Under this scheme, catalysts with a 14% nickel charge were prepared using three preparation methods: pC0: characteristics: hydrolysis and acid peptization with HNO3. A1C0: characteristics: thermal decomposition. A1C0H: characteristics: thermal decomposition and subsequent hydrothermal treatment.To sum up, three Ni-A12O3 catalysts, three Ni-Rh-A12O3 catalysts, and three Ni-Ru-A12O3 catalysts were prepared.Each catalyst was prepared using the three methods: pC0-Ni-X, A1C0-Ni-X, and A1C0H-Ni-X, (X= Ru or Rh).The precursors of alumina and nickel were aluminum sec-butoxide and nickel 1-methoxide-2-propoxide. Microstructure characterization was studied by

  15. Immobilization of a Metal-Nitrogen-Carbon Catalyst on Activated Carbon with Enhanced Cathode Performance in Microbial Fuel Cells.

    Science.gov (United States)

    Yang, Wulin; Logan, Bruce E

    2016-08-23

    Applications of microbial fuel cells (MFCs) are limited in part by low power densities mainly due to cathode performance. Successful immobilization of an Fe-N-C co-catalyst on activated carbon (Fe-N-C/AC) improved the oxygen reduction reaction to nearly a four-electron transfer, compared to a twoelectron transfer achieved using AC. With acetate as the fuel, the maximum power density was 4.7±0.2 W m(-2) , which is higher than any previous report for an air-cathode MFC. With domestic wastewater as a fuel, MFCs with the Fe-N-C/AC cathode produced up to 0.8±0.03 W m(-2) , which was twice that obtained with a Pt-catalyzed cathode. The use of this Fe-N-C/AC catalyst can therefore substantially increase power production, and enable broader applications of MFCs for renewable electricity generation using waste materials.

  16. Synthesis of Dimethyl Carbonate from Ethylene Carbonate and Methanol Over Nano-Catalysts Supported on CeO2-MgO.

    Science.gov (United States)

    Jun, Jin Oh; Lee, Joongwon; Kang, Ki Hyuk; Song, In Kyu

    2015-10-01

    A series of CeO2(X)-MgO(1-X) (X = 0, 0.25, 0.5, 0.75, and 1.0) nano-catalysts were prepared by a co-precipitation method for use in the synthesis of dimethyl carbonate from ethylene carbonate and methanol. Among the CeO2(X)-MgO(1-X) catalysts, CeO2(0.25)-MgO(0.75) nano-catalyst showed the best catalytic performance. Alkali and alkaline earth metal oxides (MO = Li2O, K2O, Cs2O, SrO, and BaO) were then supported on CeO2(0.25)-MgO(0.75) by an incipient wetness impregnation method with an aim of improving the catalytic performance of CeO2(0.25)-MgO(0.75). Basicity of the catalysts was determined by CO2-TPD experiments in order to elucidate the effect of basicity on the catalytic performance. The correlation between catalytic performance and basicity showed that basicity played an important role in the reaction. Yield for dimethyl carbonate increased with increasing basicity of the catalysts. Among the catalysts tested, Li2O/CeO2(0.25)-MgO(0.75) nano-catalyst with the largest basicity showed the best catalytic performance in the synthesis of dimethyl carbonate. PMID:26726512

  17. Size and Promoter Effects on Stability of Carbon-Nanofiber-Supported Iron-Based Fischer–Tropsch Catalysts

    Science.gov (United States)

    2016-01-01

    The Fischer–Tropsch Synthesis converts synthesis gas from alternative carbon resources, including natural gas, coal, and biomass, to hydrocarbons used as fuels or chemicals. In particular, iron-based catalysts at elevated temperatures favor the selective production of C2–C4 olefins, which are important building blocks for the chemical industry. Bulk iron catalysts (with promoters) were conventionally used, but these deactivate due to either phase transformation or carbon deposition resulting in disintegration of the catalyst particles. For supported iron catalysts, iron particle growth may result in loss of catalytic activity over time. In this work, the effects of promoters and particle size on the stability of supported iron nanoparticles (initial sizes of 3–9 nm) were investigated at industrially relevant conditions (340 °C, 20 bar, H2/CO = 1). Upon addition of sodium and sulfur promoters to iron nanoparticles supported on carbon nanofibers, initial catalytic activities were high, but substantial deactivation was observed over a period of 100 h. In situ Mössbauer spectroscopy revealed that after 20 h time-on-stream, promoted catalysts attained 100% carbidization, whereas for unpromoted catalysts, this was around 25%. In situ carbon deposition studies were carried out using a tapered element oscillating microbalance (TEOM). No carbon laydown was detected for the unpromoted catalysts, whereas for promoted catalysts, carbon deposition occurred mainly over the first 4 h and thus did not play a pivotal role in deactivation over 100 h. Instead, the loss of catalytic activity coincided with the increase in Fe particle size to 20–50 nm, thereby supporting the proposal that the loss of active Fe surface area was the main cause of deactivation. PMID:27330847

  18. Carbon monoxide oxidation using Zn-Cu-Ti hydrotalcite-derived catalysts

    Indian Academy of Sciences (India)

    O Saber; T Zaki

    2014-07-01

    Multioxide catalysts of zinc, copper and titanium with different ratios obtained from layered double hydroxide (LDH) precursors were used in the oxidation of carbon monoxide. The catalysts were characterized by energy-dispersive X-ray spectrometry, X-ray diffraction, thermal analyses (TG, DTG and DTA) and scanning electron microscopy. X-ray diffraction showed different phases of double hydroxide structures. On increasing the percentage of zinc, hydrotalcite structure became the main phase in these samples. SEM images confirmed the presence of layered double hydroxide as plate-like structure. Experimental results indicated a sharp increase in the catalytic activities of the calcined samples towards the oxidation of carbon monoxide at temperatures in the range of 225-275°C. High conversion of carbon monoxide (90 ∼ 95%) was achieved at reaction temperature of 275°C by samples having ZnTiO3 as a main phase. These results suggested that hydrotalcite structure of Zn-Ti has a positive catalytic effect towards carbon monoxide oxidation.

  19. IR study on surface chemical properties of catalytic grown carbon nanotubes and nanofibers

    Institute of Scientific and Technical Information of China (English)

    Li-hua TENG; Tian-di TANG

    2008-01-01

    In this study, the surface chemical properties of carbon nanotubes (CNTs) and carbon nanofibers (CNFs) grown by catalytic decomposition of methane on nickel and cobalt based catalysts were studied by DRIFT (Diffuse Reflectance Infrared Fourier Transform) and transmission Infrared (IR) spectroscopy. The results show that the surface exists not only carbon-hydrogen groups, but also carboxyl, ketene or quinone (carbonyl) oxygen-containing groups. These functional groups were formed in the process of the material growth, which result in large amount of chemical defect sites on the walls.

  20. Covalent versus Charge Transfer Modification of Graphene/Carbon-Nanotubes with Vitamin B1: Co/N/S-C Catalyst toward Excellent Oxygen Reduction.

    Science.gov (United States)

    Vij, Varun; Tiwari, Jitendra N; Kim, Kwang S

    2016-06-29

    High-performance nonprecious cathodic catalysts for oxygen reduction are highly demanded for low-temperature polymer electrolyte membrane fuel cells (PEMFCs). Here, we report a noble-meta- free, nitrogen and sulfur codoped graphene(G)/carbon-nanotube(CNT) material decorated with Co nanoparticles (NPs), which serve as catalytic sites for excellent oxygen reduction reaction (ORR) in basic and acidic media. Out of the cathodic catalysts synthesized by either covalent (cov) or charge transfer (CT) modification of graphen oxide (GO) with thiamine (Th: Vitamin B1), ThG/CNT/Co-cov shows more promising ORR properties than ThG/CNT/Co-CT. Catalyst ThG/CNT/Co-cov exhibits onset/halfwave potentials of 0.95/0.86 V in 0.1 M KOH and 0.92/0.83 V in 0.1 M HClO4, which are comparable to those of commercial catalyst Pt/C (0.95/0.86 V). As compared to Pt/C, our catalyst shows higher current densities of 6.72 mA cm(-2) in basic medium and 7.08 mA cm(-2) in acidic medium at 0.55 V (vs reversible hydrogen electrode (RHE)). It also exhibits better catalytic stability and methanol tolerance. High catalytic efficiency and stability of ThG/CNT/Co-cov show a promising prospect of materialization of PEMFCs for clean energy production. PMID:27255326

  1. Mössbauer Spectroscopy Investigation and Hydrodesulfurization Properties of Iron–nickel Phosphide Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Gaudette, Amy F.; Burns, Autumn W.; Hayes, John R.; Smith, Mica C.; Bowker, Richard H.; Seda, Takele; Bussell, Mark E.

    2010-05-25

    Unsupported and silica-supported FexNi2-xPy catalysts having a range of metal compositions (0 < x 6 2.0) were investigated using Mössbauer spectroscopy, and the results correlated with the surface and hydrodesulfurization (HDS) properties of the supported catalysts. Mössbauer spectroscopy permits determination of the relative site occupancy of Fe atoms in tetrahedral (M(1)) and pyramidal (M(2)) sites in the FexNi2-xPy materials. Fe atoms preferentially occupy M(2) sites for materials with significant Fe contents (x > ~0.60), but the Fe site preference reverses as the Fe content decreases (x < ~0.60). Similar occupation trends are observed for the unsupported and silica-supported FexNi2-xPy materials. Thiophene HDS measurements of the FexNi2-xPy/SiO2 catalysts revealed catalysts with high Fe contents (0.80 6 x 6 2.00) to have low activities, while the activities of Ni-rich catalysts increased dramatically with increased Ni content (0.03 6 x 6 0.60). The highest HDS activity was measured for a catalyst having a nominal precursor composition of Fe0.03Ni1.97P2.00/SiO2; this catalyst was 40% more active than a optimized nickel phosphide catalyst prepared from a precursor having a nominal composition of Ni2.00P1.60/SiO2. The 25 wt.% Fe0.03Ni1.97P2.00/SiO2 catalyst also had a dibenzothiophene HDS activity just over 10% higher than that of the 25 wt.% Ni2.00P1.60/SiO2 catalyst at 548 K. The trend of increasing HDS activity for the FexNi2-xPy/ SiO2 catalysts correlates with preferential Fe occupation of M(1) sites (and, therefore, Ni occupation of M(2) sites). Supported by X-ray photoelectron spectroscopy and oxygen chemisorption measurements, we conclude that the high activity of Ni-rich FexNi2-xPy/SiO2 catalysts can be traced to a high surface density of Ni in M(2) sites that are resistant to site blockage due to S incorporation.

  2. Growing Zigzag (16,0) Carbon Nanotubes with Structure-Defined Catalysts.

    Science.gov (United States)

    Yang, Feng; Wang, Xiao; Zhang, Daqi; Qi, Kuo; Yang, Juan; Xu, Zhi; Li, Meihui; Zhao, Xiulan; Bai, Xuedong; Li, Yan

    2015-07-15

    The growth of zigzag single-walled carbon nanotubes (SWNTs) is most challenging among all types of SWNTs, with the highest reported selectivity of ∼7%. Here we realized the dominant growth of (16,0) tubes at the abundance near ∼80% by using intermetallic W6Co7 catalysts containing plenty of (1 1 6) planes together with optimizing the growth conditions. These (1 1 6) planes may act as the structure templates for (16,0) SWNTs due to the geometrical match between the open end of the (16,0) tube and the atomic arrangements of the (1 1 6) planes in W6Co7. Using catalysts with designed structure as solid state template at suitable kinetic conditions offers a strategy for selective growth of zigzag SWNTs. PMID:26125333

  3. Mesoporous nitrogen-rich carbon materials as cathode catalysts in microbial fuel cells

    KAUST Repository

    Ahn, Yongtae

    2014-12-01

    The high cost of the catalyst material used for the oxygen reduction reaction in microbial fuel cell (MFC) cathodes is one of the factors limiting practical applications of this technology. Mesoporous nitrogen-rich carbon (MNC), prepared at different temperatures, was examined as an oxygen reduction catalyst, and compared in performance to Pt in MFCs and electrochemical cells. MNC calcined at 800 °C produced a maximum power density of 979 ± 131 mW m-2 in MFCs, which was 37% higher than that produced using MNC calined at 600 °C (715 ± 152 mW m-2), and only 14% lower than that obtained with Pt (1143 ± 54 mW m-2). The extent of COD removal and coulombic efficiencies were the same for all cathode materials. These results show that MNC could be used as an alternative to Pt in MFCs. © 2014 Elsevier B.V. All rights reserved.

  4. Electro-oxidation of Ethanol on Carbon Supported PtSn and PtSnNi Catalysts

    OpenAIRE

    Nur Hidayati; Keith Scott

    2016-01-01

    Even though platinum is known as an active electro-catalyst for ethanol oxidation at low temperatures (< 100 oC), choosing the electrode material for ethanol electro-oxidation is a crucial issue. It is due to its property which easily poisoned by a strong adsorbed species such as CO. PtSn-based electro-catalysts have been identified as better catalysts for ethanol electro-oxidation. The third material is supposed to improved binary catalysts performance. This work presents a study of the etha...

  5. Highly Active Carbon Supported Pd-Ag Nanofacets Catalysts for Hydrogen Production from HCOOH.

    Science.gov (United States)

    Wang, Wenhui; He, Ting; Liu, Xuehua; He, Weina; Cong, Hengjiang; Shen, Yangbin; Yan, Liuming; Zhang, Xuetong; Zhang, Jinping; Zhou, Xiaochun

    2016-08-17

    Hydrogen is regarded as a future sustainable and clean energy carrier. Formic acid is a safe and sustainable hydrogen storage medium with many advantages, including high hydrogen content, nontoxicity, and low cost. In this work, a series of highly active catalysts for hydrogen production from formic acid are successfully synthesized by controllably depositing Pd onto Ag nanoplates with different Ag nanofacets, such as Ag{111}, Ag{100}, and the nanofacet on hexagonal close packing Ag crystal (Ag{hcp}). Then, the Pd-Ag nanoplate catalysts are supported on Vulcan XC-72 carbon black to prevent the aggregation of the catalysts. The research reveals that the high activity is attributed to the formation of Pd-Ag alloy nanofacets, such as Pd-Ag{111}, Pd-Ag{100}, and Pd-Ag{hcp}. The activity order of these Pd-decorated Ag nanofacets is Pd-Ag{hcp} > Pd-Ag{111} > Pd-Ag{100}. Particularly, the activity of Pd-Ag{hcp} is up to an extremely high value, i.e., TOF{hcp} = 19 000 ± 1630 h(-1) at 90 °C (lower limit value), which is more than 800 times higher than our previous quasi-spherical Pd-Ag alloy nanocatalyst. The initial activity of Pd-Ag{hcp} even reaches (3.13 ± 0.19) × 10(6) h(-1) at 90 °C. This research not only presents highly active catalysts for hydrogen generation but also shows that the facet on the hcp Ag crystal can act as a potentially highly active catalyst. PMID:27454194

  6. Direct synthesis of dimethyl carbonate and propylene glycol using potassium bicarbonate as catalyst in supercritical CO2

    Directory of Open Access Journals (Sweden)

    Wen Yicun

    2015-03-01

    Full Text Available The improved one-pot synthesis of dimethyl carbonate and propylene glycol from propylene oxide, supercritical carbon dioxide, and methanol with potassium bicarbonate as the catalyst has been reported in this paper. As far as we know, it is the first time to use potassium bicarbonate only as the catalyst in the production process which is simple and cheap. Satisfactory conversion rate of propylene oxide and yield of the products could be achieved at the optimized conditions with quite a small amount of by-products. Our new method offers an attractive choice for the production of dimethyl carbonate in large-scale industry efficiently and environmental friendly.

  7. Structural and Electrocatalytic Properties of PtIrCo/C Catalysts for Oxygen Reduction Reaction

    Energy Technology Data Exchange (ETDEWEB)

    Loukrakpam, Rameshwori; Wanjala, Bridgid N.; Yin, Jun; Fang, Bin; Luo, Jin; Shao, Minhua; Protsailo, Lesia; Kawamura, Tetsuo; Chen, Yongsheng; Petkov, Valeri; Zhong, Chuan-Jian (Binghamton); (Penn); (UTC Power); (Toyota); (CMU)

    2015-10-15

    This paper describes the results of an investigation of the synthesis of PtIrCo nanoparticles (2-3 nm) for electrocatalytic oxygen reduction reaction. The carbon-supported PtIrCo catalysts (PtIrCo/C) were thermally treated at temperatures ranging from 400 to 900 C. The size, composition, and atomic-scale structures of the PtIrCo/C catalysts were characterized for establishing their correlation with the electrocatalytic activity toward oxygen reduction reaction. The specific activity was found to increase by a factor of 3-5 for the PtIrCo/C catalysts in comparison with Pt/C catalysts. A correlation was identified between the specific activity and the nanoparticle's fcc-type lattice parameter. The specific activity increases whereas the fcc-type lattice parameter decreases with the thermal treatment temperature. This correlation was further substantiated by analyzing the interatomic spatial parameters in the trimetallic nanoparticles based on X-ray absorption fine structure spectroscopic and high-energy XRD experiments. Implications of these findings, along with the durability of the catalysts, to the design of active electrocatalysts were also discussed.

  8. Low-temperature SCR of NO{sub x} with NH{sub 3} over carbon-ceramic supported catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Valdes-Solis, Teresa; Marban, Gregorio; Fuertes, Antonio B. [Instituto Nacional del Carbon (CSIC), c/Francisco Pintado Fe No. 26, 33011 Oviedo (Spain)

    2003-11-10

    A new method for preparing vanadium oxide supported on carbon-ceramic cellular monoliths is described. This includes a support oxidation step with HNO{sub 3}, followed by ionic exchange with a NaOH solution, equilibrium adsorption impregnation of VO{sup 2+} and thermal treatment. As a result an active catalyst for low-temperature selective catalytic reduction (SCR) reaction is obtained. The V-catalyst is more resistant to SO{sub 2} poisoning than the previously developed Mn-catalyst. Inhibition by water is reversible for both types of catalysts. Testing of the vanadium catalyst after subjecting it to the outlet gas stream of a power plant shows fast deactivation until constant residual activity is reached. Deactivation seems to be caused by arsenic poisoning and the formation of superficial sulphates.

  9. Palladium nanoparticles on hierarchical carbon surfaces: A new architecture for robust nano-catalysts

    Science.gov (United States)

    Vijwani, Hema; Mukhopadhyay, Sharmila M.

    2012-12-01

    Surface activity of heterogeneous catalysts can be enhanced if their sizes are reduced to nanometers. However, loose nanomaterials pose potential health and environmental risks. This issue has been addressed by attachment of palladium nanoparticles on multi-scale hierarchical carbon supports that have exceptionally high surface area per volume. The supports consist of porous carbon foam whose surface has been either chemically functionalized, or morphologically altered by grafting of carbon-nanotubes. It is seen that whereas chemical functionalization does provide some increase in nano-catalyst loading, morphological modification is significantly more powerful. It has the potential to create orders of magnitude increase in catalytic activity within the same overall volume. The synthesis techniques have been investigated in sufficient detail to provide significant control over the density and size of nanoparticles. Abundant distribution of nanoparticles is observed even within the deeper pores of the microcellular foam. The nanoparticles are seen to be metallic Pd having face centered cubic structure. Additionally, the nano-particles and nanotubes are durable, and remain attached to the base support after long periods of rapid rotation in water. These robust hybrid structures show promise in future applications such as sensors, water purification systems, fuel cell electrodes and hydrogen storage sponges.

  10. Carbon nanohybrids used as catalysts and emulsifiers for reactions in biphasic aqueous/organic systems

    Institute of Scientific and Technical Information of China (English)

    Daniel E. Resasco

    2014-01-01

    This mini-review summarizes some novel aspects of reactions conducted in aqueous/organic emul-sions stabilized by carbon nanohybrids functionalized with catalytic species. Carbon nanohybrids represent a family of solid catalysts that not only can stabilize water-oil emulsions in the same fash-ion as Pickering emulsions, but also catalyze reactions at the liquid/liquid interface. Several exam-ples are discussed in this mini-review. They include (a) aldol condensation-hydrodeoxygenation tandem reactions catalyzed by basic (MgO) and metal (Pd) catalysts, respectively; (b) Fischer-Tropsch synthesis catalyzed by carbon-nanotube-supported Ru;and (c) emulsion polymerization of styrene for the production of conductive polymer composites. Conducting these reactions in emul-sion generates important advantages, such as increased liquid/liquid interfacial area that conse-quently means faster mass transfer rates of molecules between the two phases, effective separation of products from the reaction mixture by differences in the water-oil solubility, and significant changes in product selectivity that can be adjusted by modifying the emulsion characteristics.

  11. Synthesis of Nitrogen-Doped Carbon Nanocoils with Adjustable Morphology using Ni–Fe Layered Double Hydroxides as Catalyst Precursors

    Directory of Open Access Journals (Sweden)

    Tomohiro Iwasaki

    2015-01-01

    Full Text Available Nitrogen-doped carbon nanocoils (CNCs with adjusted morphologies were synthesized in a one-step catalytic chemical vapour deposition (CVD process using acetoni‐ trile as the carbon and nitrogen source. The nickel iron oxide/nickel oxide nanocomposites, which were derived from nickel–iron layered double hydroxide (LDH precur‐ sors, were employed as catalysts for the synthesis of CNCs. In this method, precursor-to-catalyst transformation, catalyst activation, formation of CNCs, and nitrogen doping were all performed in situ in a single process. The morphology (coil diameter, coil pitch, and fibre diameter and nitrogen content of the synthesized CNCs was indi‐ vidually adjusted by modulation of the catalyst composi‐ tion and CVD reaction temperature, respectively. The adjustable ranges of the coil diameter, coil pitch, fibre diameter, and nitrogen content were confirmed to be approximately 500±100 nm, 600±100 nm, 100±20 nm, and 1.1±0.3 atom%, respectively.

  12. Heterogeneous catalytic ozonation of ciprofloxacin in water with carbon nanotube supported manganese oxides as catalyst

    International Nuclear Information System (INIS)

    Highlights: ► Ciprofloxacin in water was degraded by heterogeneous catalytic ozonation. ► MnOx were supported on MWCNTs to serve as catalyst for ozonation. ► MnOx/MWCNT exhibited highly catalytic activity on ozonation of ciprofloxacin in water. ► MnOx/MWCNT resulted in effective antibacterial activity inhibition on ciprofloxacin. ► MnOx/MWCNT promoted the generation of hydroxyl radicals. - Abstract: Carbon nanotube-supported manganese oxides (MnOx/MWCNT) were used as catalysts to assist ozone in degrading ciprofloxacin in water. Manganese oxides were successfully loaded on multi-walled carbon nanotube surfaces by simply impregnating the carbon nanotube with permanganate solution. The catalytic activities of MnOx/MWCNT in ciprofloxacin ozonation, including degradation, mineralization effectiveness, and antibacterial activity change, were investigated. The presence of MnOx/MWCNT significantly elevated the degradation and mineralization efficiency of ozone on ciprofloxacin. The microbiological assay with a reference Escherichia coli strain indicated that ozonation with MnOx/MWCNT results in more effective antibacterial activity inhibition of ciprofloxacin than that in ozonation alone. The effects of catalyst dose, initial ciprofloxacin concentration, and initial pH conditions on ciprofloxacin ozonation with MnOx/MWCNT were surveyed. Electron spin resonance trapping was applied to assess the role of MnOx/MWCNT in generating hydroxyl radicals (HO·) during ozonation. Stronger 5,5-dimethyl-1-pyrroline-N-oxide–OH signals were observed in the ozonation with MnOx/MWCNT compared with those in ozonation alone, indicating that MnOx/MWCNT promoted the generation of hydroxyl radicals. The degradation of ciprofloxacin was studied in drinking water and wastewater process samples to gauge the potential effects of water background matrix on MnOx/MWCNT catalytic ozonation.

  13. Heterogeneous catalytic ozonation of ciprofloxacin in water with carbon nanotube supported manganese oxides as catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Sui, Minghao, E-mail: suiminghao.sui@gmail.com [State Key Laboratory of Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092 (China); Xing, Sichu; Sheng, Li; Huang, Shuhang; Guo, Hongguang [State Key Laboratory of Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092 (China)

    2012-08-15

    Highlights: Black-Right-Pointing-Pointer Ciprofloxacin in water was degraded by heterogeneous catalytic ozonation. Black-Right-Pointing-Pointer MnOx were supported on MWCNTs to serve as catalyst for ozonation. Black-Right-Pointing-Pointer MnOx/MWCNT exhibited highly catalytic activity on ozonation of ciprofloxacin in water. Black-Right-Pointing-Pointer MnOx/MWCNT resulted in effective antibacterial activity inhibition on ciprofloxacin. Black-Right-Pointing-Pointer MnOx/MWCNT promoted the generation of hydroxyl radicals. - Abstract: Carbon nanotube-supported manganese oxides (MnOx/MWCNT) were used as catalysts to assist ozone in degrading ciprofloxacin in water. Manganese oxides were successfully loaded on multi-walled carbon nanotube surfaces by simply impregnating the carbon nanotube with permanganate solution. The catalytic activities of MnOx/MWCNT in ciprofloxacin ozonation, including degradation, mineralization effectiveness, and antibacterial activity change, were investigated. The presence of MnOx/MWCNT significantly elevated the degradation and mineralization efficiency of ozone on ciprofloxacin. The microbiological assay with a reference Escherichia coli strain indicated that ozonation with MnOx/MWCNT results in more effective antibacterial activity inhibition of ciprofloxacin than that in ozonation alone. The effects of catalyst dose, initial ciprofloxacin concentration, and initial pH conditions on ciprofloxacin ozonation with MnOx/MWCNT were surveyed. Electron spin resonance trapping was applied to assess the role of MnOx/MWCNT in generating hydroxyl radicals (HO{center_dot}) during ozonation. Stronger 5,5-dimethyl-1-pyrroline-N-oxide-OH signals were observed in the ozonation with MnOx/MWCNT compared with those in ozonation alone, indicating that MnOx/MWCNT promoted the generation of hydroxyl radicals. The degradation of ciprofloxacin was studied in drinking water and wastewater process samples to gauge the potential effects of water background matrix on

  14. Thermostability, Photoluminescence, and Electrical Properties of Reduced Graphene Oxide–Carbon Nanotube Hybrid Materials

    Directory of Open Access Journals (Sweden)

    Fuchi Liu

    2013-01-01

    Full Text Available Reduced graphene oxide–carbon nanotube (RGO–CNT hybrid materials were prepared by a simple catalyst-free route. The thermostability, photoluminescence (PL and electrical properties of RGO–CNTs were investigated systematically. The results revealed that compared to RGO, RGO–CNTs showed multicolor PL, and higher thermostability and conductivity. The RGO–CNTs therefore have important potential applications in the fields of photonic and electrical devices.

  15. Thermostability, Photoluminescence, and Electrical Properties of Reduced Graphene Oxide–Carbon Nanotube Hybrid Materials

    OpenAIRE

    Fuchi Liu; Yong Cao; Mingdong Yi; Linghai Xie; Wei Huang; Nujiang Tang; Wei Zhong; Youwei Du

    2013-01-01

    Reduced graphene oxide–carbon nanotube (RGO–CNT) hybrid materials were prepared by a simple catalyst-free route. The thermostability, photoluminescence (PL) and electrical properties of RGO–CNTs were investigated systematically. The results revealed that compared to RGO, RGO–CNTs showed multicolor PL, and higher thermostability and conductivity. The RGO–CNTs therefore have important potential applications in the fields of photonic and electrical devices.

  16. Oxidation of CO and Methanol on Pd-Ni Catalysts Supported on Different Chemically-Treated Carbon Nanofibers

    Directory of Open Access Journals (Sweden)

    Juan Carlos Calderón

    2016-10-01

    Full Text Available In this work, palladium-nickel nanoparticles supported on carbon nanofibers were synthesized, with metal contents close to 25 wt % and Pd:Ni atomic ratios near to 1:2. These catalysts were previously studied in order to determine their activity toward the oxygen reduction reaction. Before the deposition of metals, the carbon nanofibers were chemically treated in order to generate oxygen and nitrogen groups on their surface. Transmission electron microscopy analysis (TEM images revealed particle diameters between 3 and 4 nm, overcoming the sizes observed for the nanoparticles supported on carbon black (catalyst Pd-Ni CB 1:2. From the CO oxidation at different temperatures, the activation energy Eact for this reaction was determined. These values indicated a high tolerance of the catalysts toward the CO poisoning, especially in the case of the catalysts supported on the non-chemically treated carbon nanofibers. On the other hand, apparent activation energy Eap for the methanol oxidation was also determined finding—as a rate determining step—the COads diffusion to the OHads for the catalysts supported on carbon nanofibers. The results here presented showed that the surface functional groups only play a role in the obtaining of lower particle sizes, which is an important factor in the obtaining of low CO oxidation activation energies.

  17. Direct Synthesis of Phenol from Benzene on an Activated Carbon Catalyst Treated with Nitric Acid

    Institute of Scientific and Technical Information of China (English)

    Cui-hong Chen; Jia-quan Xu; Ming-ming Jin; Gui-ying Li; Chang-wei Hu

    2011-01-01

    Commercially available coal-based activated carbon was treated by nitric acid with different concentrations and the resultant samples were used as catalysts for the direct hydroxylation of benzene to phenol in acetonitrile. Boehm titration, X-ray photoelectron spectroscopy,scanning electron microscope coupled with an energy dispersive X-ray microanalyzer, and Brunauer-Emmett-Teller method were used to characterize toe samples. The number of carboxyl groups on the surface was found to be the main factor affecting the catalytic activity. An optimum catalytic performance with a yield of 15.7% and a selectivity of 87.2% to phenol was obtained.

  18. Synthesis of single-walled carbon nanotubes by the vertical floating catalyst method

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    The vertical floating catalyst method is first used to produce single-walled carbon nanotubes (SWNTs)continuously on a large scale by a newly developed technique and pyrolysis of n-hexane. Diameter distributions, microstructure and purity of the SWNTs film, rope and web are measured by Raman spectroscopy and electron microscope.The results show that SWNTs product has a high degree of orientation, a wide distribution of diameters (0.7-2.0 nm)and high purity of > 80%.``

  19. Influence of hydrogen on chemical vapour synthesis of different carbon nanostructures using propane as precursor and nickel as catalyst

    Indian Academy of Sciences (India)

    R K Sahoo; H Mamgain; C Jacob

    2014-10-01

    The role of hydrogen in the catalytic chemical vapour deposition of carbon nanotubes using sputtered nickel thin film as a catalyst is explained in this work. The growth of different carbon nanostructures with the variation in the precursor gas content was studied by keeping all other process parameters constant and using sputtered Ni thin film as a catalyst. The catalyst granule size, its external morphology and the resulting products were analysed. Carbon nanotubes (CNTs), carbon nanofibres (CNFs) and carbon nanoribbons (CNRs) were observed under different growth conditions. The different conditions of growth leading to form tubes, fibres or ribbons were analysed by varying the flow ratio of propane and hydrogen gas during the high temperature growth. Scanning and transmission electron microscopies confirmed the above structures under different growth conditions. The role of hydrogen on the surface passivation behaviour of the Ni catalyst and its correlative effect on the growth of carbon nanostructures is analysed. This direct approach can, in principle, be used to synthesize different types of carbon nanostructures by tailoring the hydrogen concentration.

  20. Plasma coating formed TIO2 catalysts usage in cleaning the air from nitrogen oxides and carbon monoxide

    OpenAIRE

    Vitalij Kolodynskij; Pranas Baltrėnas

    2015-01-01

    The present catalytic air purification device–air cleaning device is capable to reduce nitrogen oxide sand carbon monoxide concentrations in polluted air stream and to achieve high cleaning efficiency. The principle of operation of catalytic air cleaning device is based on plasma coating formed catalysts usage. At high temperatures and oxygen concentrations in the experimental device channel, catalysts become active and reactions of conversion of pollutants start. In this research, the effici...

  1. Development of a ruthenium/phosphite catalyst system for domino hydroformylation-reduction of olefins with carbon dioxide.

    Science.gov (United States)

    Liu, Qiang; Wu, Lipeng; Fleischer, Ivana; Selent, Detlef; Franke, Robert; Jackstell, Ralf; Beller, Matthias

    2014-06-01

    An efficient domino ruthenium-catalyzed reverse water-gas-shift (RWGS)-hydroformylation-reduction reaction of olefins to alcohols is reported. Key to success is the use of specific bulky phosphite ligands and triruthenium dodecacarbonyl as the catalyst. Compared to the known ruthenium/chloride system, the new catalyst allows for a more efficient hydrohydroxymethylation of terminal and internal olefins with carbon dioxide at lower temperature. Unwanted hydrogenation of the substrate is prevented. Preliminary mechanism investigations uncovered the homogeneous nature of the active catalyst and the influence of the ligand and additive in individual steps of the reaction sequence. PMID:24811949

  2. Direct Fabrication of Carbon Nanotubes STM Tips by Liquid Catalyst-Assisted Microwave Plasma-Enhanced Chemical Vapor Deposition

    Directory of Open Access Journals (Sweden)

    Fa-Kuei Tung

    2009-01-01

    Full Text Available Direct and facile method to make carbon nanotube (CNT tips for scanning tunneling microscopy (STM is presented. Cobalt (Co particles, as catalysts, are electrochemically deposited on the apex of tungsten (W STM tip for CNT growth. It is found that the quantity of Co particles is well controlled by applied DC voltage, concentration of catalyst solution, and deposition time. Using optimum growth condition, CNTs are successfully synthesized on the tip apex by catalyst-assisted microwave-enhanced chemical vapor deposition (CA-MPECVD. A HOPG surface is clearly observed at an atomic scale using the present CNT-STM tip.

  3. 197Au Moessbauer study of the deactivation and reactivation of a carbon-supported AuCl4- hydrochlorination catalyst

    International Nuclear Information System (INIS)

    Acetylene hydrochlorination catalysts consisting of activated carbon impregnated with a solution of HAuCl4.xH2O in aqua regia have been studied by 197Au Moessbauer spectroscopy. The relative amounts of AuCl4-, of Au(0), and of an Au(I) species formed under certain process conditions were determined quantitatively. Deactivation of the catalyst at low and high temperatures was shown to be due to different mechanisms, and the reactivation of the catalyst by Cl2 gas was studied. (orig.)

  4. Deactivation of carbon supported palladium catalyst in direct formic acid fuel cell

    International Nuclear Information System (INIS)

    A new carbon black supported palladium catalyst for direct formic acid fuel cell applications has been prepared and characterized by X-ray diffraction. Bi-modal distribution of Pd crystallite sizes was observed. The average Pd size for crystallites in small size and large size ranges were about 2.7 nm and 11.2 nm, respectively. The initial activity of the catalyst in the oxidation of formic acid tested in a fuel cell was similar to a commercial well dispersed 20 wt.% Pd/Vulcan. The rates of the fuel cell power decay were measured for formic acid of two purities for various current loadings. The results showed that various mechanisms contribute to the decrease of cell power with time. In direct formic acid fuel cell (DFAFC) fed with a very pure HCOOH accumulation of CO2 gas bubbles in anode catalyst layer is responsible for observed power decay. In DFAFC fed with a pure for analysis (p.a.) grade formic acid the formation of COads poison from the formic acid impurities is the main deactivation reason.

  5. Efficient Dual-Site Carbon Monoxide Electro-Catalysts via Interfacial Nano-Engineering

    Science.gov (United States)

    Liu, Zhen; Huang, Zhongyuan; Cheng, Feifei; Guo, Zhanhu; Wang, Guangdi; Chen, Xu; Wang, Zhe

    2016-09-01

    Durable, highly efficient, and economic sound electrocatalysts for CO electrooxidation (COE) are the emerging key for wide variety of energy solutions, especially fuel cells and rechargeable metal‑air batteries. Herein, we report the novel system of nickel‑aluminum double layered hydroxide (NiAl-LDH) nanoplates on carbon nanotubes (CNTs) network. The formulation of such complexes system was to be induced through the assistance of gold nanoparticles in order to form dual-metal active sites so as to create a extended Au/NiO two phase zone. Bis (trifluoromethylsulfonyl)imide (NTf2) anion of ionic liquid electrolyte was selected to enhance the CO/O2 adsorption and to facilitate electro-catalyzed oxidation of Ni (OH)2 to NiOOH by increasing the electrophilicity of catalytic interface. The resulting neutral catalytic system exhibited ultra-high electrocatalytic activity and stability for CO electrooxidation than commercial and other reported precious metal catalysts. The turnover frequency (TOF) of the LDH-Au/CNTs COE catalyst was much higher than the previous reported other similar electrocatalysts, even close to the activity of solid-gas chemical catalysts at high temperature. Moreover, in the long-term durability testing, the negligible variation of current density remains exsisting after 1000 electrochemistry cycles.

  6. Alcohol Synthesis over Pre-Reduced Activated Carbon-Supported Molybdenum-Based Catalysts

    Directory of Open Access Journals (Sweden)

    Edwin L. Kugler

    2003-01-01

    Full Text Available Activated carbon (AC-supported molybdenum catalysts, either with or without a potassium promoter, were prepared by the incipient wetness impregnation method. The materials were characterized using differential thermal analysis (DTA and temperature programmed reduction (TPR, and were used for mixed alcohol synthesis from syngas (CO+H2. DTA results showed that a new phase, related to the interaction between Mo species and the AC support, is formed during the calcination of the Mo/AC catalyst, and the introduction of a K promoter has noticeable effect on the interaction. TPR results indicated that the Mo is more difficult to reduce after being placed onto the AC support, and the addition of a K promoter greatly promotes the formation of Mo species reducible at relatively low temperatures, while it retards the generation of Mo species that are reducible only at higher temperatures. These differences in the reduction behavior of the catalysts are atributed to the interaction between the active components (Mo and K and the support. Potassium-doping significantly promotes the formation of alcohols at the expense of CO conversion, especially to hydrocarbons. It is postulated that Mo species with intermediate valence values (averaged around +3.5 are more likely to be the active phase(s for alcohol synthesis from CO hydrogenation, while those with lower Mo valences are probably responsible for the production of hydrocarbons.

  7. Carbon monoxide oxidation over three different states of copper: Development of a model metal oxide catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Jernigan, G G [California Univ., Berkeley, CA (United States). Dept. of Chemistry

    1994-10-01

    Carbon monoxide oxidation was performed over the three different oxidation states of copper -- metallic (Cu), copper (I) oxide (Cu{sub 2}O), and copper (II) oxide (CuO) as a test case for developing a model metal oxide catalyst amenable to study by the methods of modern surface science and catalysis. Copper was deposited and oxidized on oxidized supports of aluminum, silicon, molybdenum, tantalum, stainless steel, and iron as well as on graphite. The catalytic activity was found to decrease with increasing oxidation state (Cu > Cu{sub 2}O > CuO) and the activation energy increased with increasing oxidation state (Cu, 9 kcal/mol < Cu{sub 2}O, 14 kcal/mol < CuO, 17 kcal/mol). Reaction mechanisms were determined for the different oxidation states. Lastly, NO reduction by CO was studied. A Cu and CuO catalyst were exposed to an equal mixture of CO and NO at 300--350 C to observe the production of N{sub 2} and CO{sub 2}. At the end of each reaction, the catalyst was found to be Cu{sub 2}O. There is a need to study the kinetics of this reaction over the different oxidation states of copper.

  8. Efficient Dual-Site Carbon Monoxide Electro-Catalysts via Interfacial Nano-Engineering.

    Science.gov (United States)

    Liu, Zhen; Huang, Zhongyuan; Cheng, Feifei; Guo, Zhanhu; Wang, Guangdi; Chen, Xu; Wang, Zhe

    2016-01-01

    Durable, highly efficient, and economic sound electrocatalysts for CO electrooxidation (COE) are the emerging key for wide variety of energy solutions, especially fuel cells and rechargeable metal-air batteries. Herein, we report the novel system of nickel-aluminum double layered hydroxide (NiAl-LDH) nanoplates on carbon nanotubes (CNTs) network. The formulation of such complexes system was to be induced through the assistance of gold nanoparticles in order to form dual-metal active sites so as to create a extended Au/NiO two phase zone. Bis (trifluoromethylsulfonyl)imide (NTf2) anion of ionic liquid electrolyte was selected to enhance the CO/O2 adsorption and to facilitate electro-catalyzed oxidation of Ni (OH)2 to NiOOH by increasing the electrophilicity of catalytic interface. The resulting neutral catalytic system exhibited ultra-high electrocatalytic activity and stability for CO electrooxidation than commercial and other reported precious metal catalysts. The turnover frequency (TOF) of the LDH-Au/CNTs COE catalyst was much higher than the previous reported other similar electrocatalysts, even close to the activity of solid-gas chemical catalysts at high temperature. Moreover, in the long-term durability testing, the negligible variation of current density remains exsisting after 1000 electrochemistry cycles. PMID:27650532

  9. Bifunctional catalysts based on m-phenylene-bridged porphyrin dimer and trimer platforms: synthesis of cyclic carbonates from carbon dioxide and epoxides.

    Science.gov (United States)

    Maeda, Chihiro; Taniguchi, Tomoya; Ogawa, Kanae; Ema, Tadashi

    2015-01-01

    Highly active bifunctional diporphyrin and triporphyrin catalysts were synthesized through Stille coupling reactions. As compared with a porphyrin monomer, both exhibited improved catalytic activities for the reaction of CO2 with epoxides to form cyclic carbonates, because of the multiple catalytic sites which cooperatively activate the epoxide. Catalytic activities were carefully investigated by controlling temperature, reaction time, and catalyst loading, and very high turnover number and turnover frequency were obtained: 220 000 and 46 000 h(-1) , respectively, for the magnesium catalyst, and 310 000 and 40 000 h(-1) , respectively, for the zinc catalyst. Results obtained with a zinc/free-base hybrid diporphyrin catalyst demonstrated that the Br(-) ions on the adjacent porphyrin moiety also function as nucleophiles.

  10. Synthesis of High-quality Single- and Double-walled Carbon Nanotubes on Fe/MgO Catalysts

    Directory of Open Access Journals (Sweden)

    Mehran B. Kashi

    2016-06-01

    Full Text Available In this study, Fe/MgO catalysts with three different iron contents (5, 10, and 15 wt.% were prepared by three catalyst preparation methods: impregnation, solution combustion synthesis, and co-calcination of metal ni‐ trates. The resulting catalysts were subjected to methane at 900°C in order to grow carbon nanotubes (CNTs. The powders and products were then studied by X-ray diffraction (XRD, differential thermal analysis (DTA, scanning and transmission electron microscopy (SEM and TEM, and Raman spectroscopy. Formation of MgFe2O4 upon heating the catalysts to 900°C was confirmed by XRD. After the growth step, corresponding peaks of MgFe2O4 disappeared and metallic iron peaks appeared, indicating that MgFe2O4 is the responsible phase for production of iron nanoparticles. HRTEM images showed that the product on the 5 wt.% catalysts was mostly SWNTs and DWNTs with no evidence of carbon nanofi‐ bres or multi-walled carbon nanotubes on the co-calcina‐ tion catalyst. Furthermore, ID/IG ratios obtained from Raman spectra were all below 0.1, except for one sample, showing the good quality of the products.

  11. Mechanical properties of functionalized carbon nanotubes

    International Nuclear Information System (INIS)

    Carbon nanotubes (CNTs) used to reinforce polymer matrix composites are functionalized to form covalent bonds with the polymer in order to enhance the CNT/polymer interfaces. These bonds destroy the perfect atomic structures of a CNT and degrade its mechanical properties. We use atomistic simulations to study the effect of hydrogenization on the mechanical properties of single-wall carbon nanotubes. The elastic modulus of CNTs gradually decreases with the increasing functionalization (percentage of C-H bonds). However, both the strength and ductility drop sharply at a small percentage of functionalization, reflecting their sensitivity to C-H bonds. The cluster C-H bonds forming two rings leads to a significant reduction in the strength and ductility. The effect of carbonization has essentially the same effect as hydrogenization

  12. Magnetic properties of pelagic marine carbonates

    Science.gov (United States)

    Roberts, Andrew P.; Florindo, Fabio; Chang, Liao; Heslop, David; Jovane, Luigi; Larrasoaña, Juan C.

    2013-12-01

    Pelagic carbonates are deposited far from continents, usually at water depths of 3000-6000 m, at rates below 10 cm/kyr, and are a globally important sediment type. Recent advances, with recognition of widespread preservation of biogenic magnetite (the inorganic remains of magnetotactic bacteria), have fundamentally changed our understanding of the magnetic properties of pelagic carbonates. We review evidence for the magnetic minerals typically preserved in pelagic carbonates, the effects of magnetic mineral diagenesis on paleomagnetic and environmental magnetic records of pelagic carbonates, and what magnetic properties can tell us about the open-ocean environments in which pelagic carbonates are deposited. We also discuss briefly late diagenetic remagnetisations recorded by some carbonates. Despite recent advances in our knowledge of these phenomena, much remains undiscovered. We are only at early stages of understanding how biogenic magnetite gives rise to paleomagnetic signals in sediments and whether it carries a poorly understood biogeochemical remanent magnetisation. Recently developed techniques have potential for testing how different magnetotactic bacterial species, which produce different magnetite morphologies, respond to changing nutrient and oxygenation conditions. Future work needs to test whether it is possible to develop proxies for ancient nutrient conditions from well-calibrated modern magnetotactic bacterial occurrences. A tantalizing link between giant magnetofossils and Paleogene hyperthermal events needs to be tested; much remains to be learned about the relationship between climate and the organisms that biomineralised these large and novel magnetite morphologies. Rather than being a well-worn subject that has been studied for over 60 years, the magnetic properties of pelagic carbonates hold many secrets that await discovery.

  13. Physical properties of molten carbonate electrolyte

    Energy Technology Data Exchange (ETDEWEB)

    Kojima, T.; Yanagida, M.; Tanimoto, K. [Osaka National Research Institute (Japan)] [and others

    1996-12-31

    Recently many kinds of compositions of molten carbonate electrolyte have been applied to molten carbonate fuel cell in order to avoid the several problems such as corrosion of separator plate and NiO cathode dissolution. Many researchers recognize that the addition of alkaline earth (Ca, Sr, and Ba) carbonate to Li{sub 2}CO{sub 3}-Na{sub 2}CO{sub 3} and Li{sub 2}CO{sub 3}-K{sub 2}CO{sub 3} eutectic electrolytes is effective to avoid these problems. On the other hand, one of the corrosion products, CrO{sub 4}{sup 2-} ion is found to dissolve into electrolyte and accumulated during the long-term MCFC operations. This would affect the performance of MCFC. There, however, are little known data of physical properties of molten carbonate containing alkaline earth carbonates and CrO{sub 4}{sup 2-}. We report the measured and accumulated data for these molten carbonate of electrical conductivity and surface tension to select favorable composition of molten carbonate electrolytes.

  14. Hydrodechlorination of 4-chlorophenol in water with formic acid using a Pd/activated carbon catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Calvo, L.; Gilarranz, M.A.; Casas, J.A.; Mohedano, A.F. [Seccion de Ingenieria Quimica, Facultad de Ciencias, Universidad Autonoma de Madrid, Cantoblanco, 28049 Madrid (Spain); Rodriguez, J.J. [Seccion de Ingenieria Quimica, Facultad de Ciencias, Universidad Autonoma de Madrid, Cantoblanco, 28049 Madrid (Spain)], E-mail: juanjo.rodriguez@uam.es

    2009-01-30

    This work reports on the feasibility of hydrodechlorination as a treatment technique for chlorophenols-bearing wastewaters using formic acid as a hydrogen source. 4-Chlorophenol (4-CPhOH) has been used as target compound and the experiments were carried out in batch and continuous mode with a commercial activated carbon-supported Pd (0.5 wt.%) catalyst. The variables studied in the batch runs were HCOOH/4-CPhOH molar ratio (10-1000), temperature (25-75 deg. C) and catalyst concentration (250-1000 mg/L). The continuous experiments were performed in a fixed bed reactor where aqueous solutions of formic acid and 4-CPhOH with molar ratios between 50 and 100 were continuously fed to the reactor, at different space-time values in the range of 10.7-42.8 kg{sub cat} h/mol. Reaction temperatures from 35 to 100 deg. C were tested and the pressure was fixed at 2.5 bar. Conversion values above 99% for 4-CPhOH were obtained in batch experiments, but using a HCOOH/4-CPhOH molar ratio as high as 500. Moreover, most of the phenol produced was adsorbed on the catalyst. Continuous runs were performed to evaluate the efficiency of the catalyst under lower HCOOH/4-CPhOH ratios and to explore the possibility of converting phenol to more hydrogenated products. The results indicated that the HCOOH/4-CPhOH molar ratios needed were an order of magnitude lower than those required in batch runs to achieve conversions of 4-CPhOH close to 95%. Besides, phenol was not the only reaction product formed, since a more hydrogenated product such as cyclohexanone was detected in the effluent, which indicates additional hydrogenation of phenol in contrast to the behaviour observed in batch experiments. A loss of activity was observed in the continuous runs after 20-30 h on stream.

  15. Ferromagnetic Property and Synthesis of Onion-Like Fullerenes by Chemical Vapor Deposition Using Fe and Co Catalysts Supported on NaCl

    International Nuclear Information System (INIS)

    Metal-encapsulating onion-like fullerenes (MOLFs) were synthesized by CVD at relatively low temperature (420 degree C) using Fe and Co nanoparticles impregnated into NaCl as catalyst. The morphology and structure of the products were characterized by field emission scanning electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and Raman spectroscopy. The results show that Fe OLFs and Co OLFs with stacked graphitic fragments were prepared using Fe/NaCl or Co/NaCl as catalysts; after Co OLFs were immersed in concentrated HCl for 48 hours, Co nanoparticles encapsulated by carbon shells were not removed, meaning that carbon shells can protect the encapsulated Co cores against environmental degradation. The coercivity value (750.23 Oe) of Co OLFs showed an obvious magnetic property.

  16. Ferromagnetic Property and Synthesis of Onion-Like Fullerenes by Chemical Vapor Deposition Using Fe and Co Catalysts Supported on NaCl

    Directory of Open Access Journals (Sweden)

    Yongzhen Yang

    2011-01-01

    Full Text Available Metal-encapsulating onion-like fullerenes (M@OLFs were synthesized by CVD at relatively low temperature (420C∘ using Fe and Co nanoparticles impregnated into NaCl as catalyst. The morphology and structure of the products were characterized by field emission scanning electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and Raman spectroscopy. The results show that Fe@OLFs and Co@OLFs with stacked graphitic fragments were prepared using Fe/NaCl or Co/NaCl as catalysts; after Co@OLFs were immersed in concentrated HCl for 48 hours, Co nanoparticles encapsulated by carbon shells were not removed, meaning that carbon shells can protect the encapsulated Co cores against environmental degradation. The coercivity value (750.23 Oe of Co@OLFs showed an obvious magnetic property.

  17. Caesium carbonate as a highly efficient catalyst for the synthesis of macrocyclicdiamides

    Directory of Open Access Journals (Sweden)

    Esmael Rostami

    2014-07-01

    Full Text Available In this research work, we report the synthesis of macrocyclicdiamides from the reaction of diesters and aliphatic diamines in the presence of caesium carbonate. It has been demonstrated that among the carbonate of alkali metals (Li2CO3, Na2CO3, K2CO3 and CS2CO3, CS2CO3 appears to be the best catalyst for macrocyclization. Diesters with different substitution patterns on the aromatic ring reacted smoothly with diamines under optimal conditions, affording the corresponding macrocycles in high yields. Introducing a rigid group (e.g., sulfone on the substrate led to somewhat decreased yield. Various substrates proved to be suitable for this macrocyclization reaction, especially, the flexible ones.

  18. Effect of solvent on Se-modified ruthenium/carbon catalyst for oxygen reduction

    Directory of Open Access Journals (Sweden)

    Chuanxiang Zhang

    2014-12-01

    Full Text Available Se-modified ruthenium supporting on carbon (Sex–Ru/C electrocatalyst was prepared by solvothermal one-step synthesis method. The reaction mechanism was revealed after discussing impact of different solvents (i-propanol and EG in solvotermal reaction. The result showed that the grain size of Se-modified ruthenium electrocatalyst was as small as 1 to 3 nm and highly dispersed on carbon surface. X-ray photoelectron spectroscopy (XPS presented that selenium mainly existed in the catalyst in the form of elemental selenium and selenium oxides when the solvent was EG and i-propanol, respectively. The oxygen reduction reaction (ORR performance was improved by appearance of selenium oxides.

  19. Characterization and Catalytic Properties of a Rapidly Quenched Ni-RE-P-AL Catalyst

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    A Ni-RE-P-AL catalyst prepared by alkaline extraction of a rapidly quenched Ni-RE-P-AL alloy was characterized by means of ICP,BET,XRD,ZPS and TEM.The results show that the rapidly quenched Ni-RE-P-AL alloy contained less crystalline AL3Ni than AL-Ni alloy.After alkaline extraction,most of Al in the Ni-RE-P-AL alloy was leached out and the resulted Ni-RE-P-AL catalyst presented a spone structure similar to Raney Ni.Although Crystalline Ni is the major phase in the Ni-RE-P-AL catalyst and Raney Ni,amorphous Ni-P phase has been detected in the Ni-RE-P-AL catalyst.Studies on catalytic hydrogenation of toluene,phenyl ethylene,acetylene benzene,nitrobenzene,cyclohexanone and adiponitrile in liquid phase showed that the activity and selectivity of this Ni-RE-P-AL catalyst are superior to those of Raney Ni,especially at low temperatures.The amorphous phase is considered to be responsible for its superior catalytic properties.

  20. Effects of Current on Microcosmic Properties of Catalyst and Reforming of Bio-oil

    Institute of Scientific and Technical Information of China (English)

    Li-xia Yuan; Tong-qi Ye; Fei-yan Gong; Quan-xin Li

    2009-01-01

    Highly effective production of hydrogen from bio-oil was achieved by using a low-temperature electrochemical catalytic reforming approach over the conventional Ni-based reforming cat-alyst (NiO-Al2O3), where an AC electronic current passed through the catalyst bed. The promoting effects of current on the bio-oil reforming were studied. It was found that the performance of the bio-oil reforming was remarkably enhanced by the current which passed through the catalyst. The effects of currents on the microcosmic properties of the catalyst, including the Brunauer-Emmett-Teller (BET) surface area, pore diameter, pore volume, the size of the crystallites and the reduction level of NiO into Ni, were carefully characterized by BET, X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscope. The desorption of the thermal electrons from the electrified catalyst was directly observed by the TOF (time of flight) measurements. The mechanism of the electrochemical catalytic reforming of bio-oil is discussed based on the above investigation.

  1. Impact of Precipitants on the Structure and Properties of Fe-Co-Ce Composite Catalysts

    Directory of Open Access Journals (Sweden)

    Yongli Zhang

    2016-01-01

    Full Text Available Fe-Co-Ce composite catalysts were prepared by coprecipitation method using CO(NH22, NaOH, NH4HCO3, and NH3·H2O as precipitant agents. The effects of the precipitant agents on the physicochemical properties of the Fe-Co-Ce based catalysts were investigated by SEM, TEM, BET, TG-DTA, and XRD. It was found that the precipitant agents remarkably influenced the morphology and particle size of the catalysts and affected the COD removal efficiency, decolorization rate, and pH of methyl orange for catalytic wet air oxidation (CWAO. The specific surface area of the Fe-Co-Ce composite catalysts successively decreased in the order of NH3·H2O, NH4HCO3, NaOH, and CO(NH22, which correlated to an increasing particle size that increased for each catalyst. For the CWAO of a methyl orange aqueous solutions, the effects of precipitant agents NH3·H2O and NaOH were superior to those of CO(NH22 and NH4HCO3. The catalyst prepared using NH3·H2O as the precipitant agent was mostly composed of Fe2O3, CoO, and CeO2. The COD removal efficiency of methyl orange aqueous solution for NH3·H2O reached 92.9% in the catalytic wet air oxidation. Such a catalytic property was maintained for six runs.

  2. Potassium-decorated active carbon supported Co-Mo-based catalyst for water-gas shift reaction

    Institute of Scientific and Technical Information of China (English)

    Yixin Lian; RuiFen Xiao; Weiping Fang; Yiquan Yang

    2011-01-01

    The effect of potassium-decoration was studied on the activity of water-gas shift(WGS)reaction over the Co-Mo-based catalysts supported on active carbon(AC),which was prepared by incipient wetness co-impregnation method.The decoration of potassium on active carbon in advance enhances the activities of the CoMo-K/AC catalysts for WGS reaction.Highest activity(about 92% conversion)was obtained at250 ℃ for the catalyst with an optimum K2O/AC weight ratio in the range from 0.12 to 0.15.The catalysts were characterized by TPR and EPR,and the results show that activated carbon decorated with potassium makes Co-Mo species highly dispersed,and thus easily reduced and sulfurized.XRD results show that an appropriate content of potassium-decoration on active carbon supports may favors the formation of highly dispersed Co9Ss-type structures which are situated on the edge or a site in contact with MoS2,K-Mo-O-S,Mo-S-K phase.Those active species are responsible for the high activity of CoMo-K/AC catalysts.

  3. Ultrafine porous carbon fiber and its supported platinum catalyst for enhancing performance of proton exchange membrane fuel cells

    International Nuclear Information System (INIS)

    The enhancement of electrocatalytic activity of carbon-supported platinum catalysts has been essential for improving the performance of proton exchange membrane fuel cells (PEMFCs). In this paper, one kind of grounded ultrafine porous carbon fiber (UPCF), with an average diameter of the order of 100 nm and pore sizes of 5–30 nm, was used as a novel compound carbon support (CCS) to prepare a supported Pt catalyst (Pt/CCS) for the electrode catalyst layer in a PEMFC, and its associated membrane electrode assembly (MEA). The fabricated MEA was also tested in a single fuel cell to validate this Pt/CCS catalyst. The electrochemical surface area (ECSA) of Pt was determined to be 71.9 m2.g−1 for the CCS, which is much larger than the 54.6 m2.g−1 known to apply for carbon black support. Both the onset potential and half-wave potential of Pt/CCS were all positively shifted in comparison with Pt/C, based on linear sweep voltammetry (LSV). The performance of a single fuel cell catalyzed by Pt/CCS showed 1.25 times higher power density than that catalyzed by Pt/C at room temperature. The cross-sectional morphology of the electrode indicated the chopped-fiber-form UPCF might construct a loose three-dimensionally layer-like catalyst that could reduce mass transform resistance and allow the water produced to escape easily

  4. A nitrogen-doped mesoporous carbon containing an embedded network of carbon nanotubes as a highly efficient catalyst for the oxygen reduction reaction.

    Science.gov (United States)

    Li, Jin-Cheng; Zhao, Shi-Yong; Hou, Peng-Xiang; Fang, Ruo-Pian; Liu, Chang; Liang, Ji; Luan, Jian; Shan, Xu-Yi; Cheng, Hui-Ming

    2015-12-01

    A nitrogen-doped mesoporous carbon containing a network of carbon nanotubes (CNTs) was produced for use as a catalyst for the oxygen reduction reaction (ORR). SiO2 nanoparticles were decorated with clusters of Fe atoms to act as catalyst seeds for CNT growth, after which the material was impregnated with aniline. After polymerization of the aniline, the material was pyrolysed and the SiO2 was removed by acid treatment. The resulting carbon-based hybrid also contained some Fe from the CNT growth catalyst and was doped with N from the aniline. The Fe-N species act as active catalytic sites and the CNT network enables efficient electron transport in the material. Mesopores left by the removal of the SiO2 template provide short transport pathways and easy access to ions. As a result, the catalyst showed not only excellent ORR activity, with 59 mV more positive onset potential and 30 mV more positive half-wave potential than a Pt/C catalyst, but also much longer durability and stronger tolerance to methanol crossover than a Pt/C catalyst.

  5. Novel growth method of carbon nanotubes using catalyst-support layer developed by alumina grit blasting.

    Science.gov (United States)

    Watanabe, Hiromichi; Ishii, Juntaro; Ota, Keishin

    2016-08-19

    We propose an efficient method of growing carbon nanotube (CNT) arrays on a variety of metals, alloys, and carbon materials using chemical vapor deposition (CVD) assisted by a simple surface treatment of the materials. The main feature of this method is the application of grit blasting with fine alumina particles to the development of a catalyst-support layer required for the growth of CNTs on various conductive materials, including ultra-hard metals such as tungsten. Auger electron spectroscopy shows that grit blasting can form a non-continuous layer where alumina nanoparticles are embedded as residues in the blasting media left on the treated surfaces. This work reveals that such a non-continuous alumina layer can behave as the catalyst-support layer, which is generally prepared by sputter or a vacuum evaporation coating process that considerably restricts the practical applications of CNTs. We have attempted to grow CNTs on grit-blasted substrates of eighteen conventionally used conductive materials using CVD together with a floating iron catalyst. The proposed method was successful in growing multi-walled CNT arrays on the grit-blasted surfaces of all the examined materials, demonstrating its versatility. Furthermore, we found that the group IV metal oxide films thermally grown on the as-received substrates can support the catalytic activity of iron nanoparticles in the CVD process just as well as the alumina film developed by grit blasting. Spectral emissivity of the CNT arrays in the visible and infrared wavelength ranges has been determined to assess the applicability of the CNT arrays as a black coating media. PMID:27389659

  6. Amorphous Molybdenum Sulfide on Graphene-Carbon Nanotube Hybrids as Highly Active Hydrogen Evolution Reaction Catalysts.

    Science.gov (United States)

    Pham, Kien-Cuong; Chang, Yung-Huang; McPhail, David S; Mattevi, Cecilia; Wee, Andrew T S; Chua, Daniel H C

    2016-03-01

    In this study, we report on the deposition of amorphous molybdenum sulfide (MoSx, with x ≈ 3) on a high specific surface area conductive support of Graphene-Carbon Nanotube hybrids (GCNT) as the Hydrogen Evolution Reaction (HER) catalysts. We found that the high surface area GCNT electrode could support the deposition of MoSx at much higher loadings compared with simple porous carbon paper or flat graphite paper. The morphological study showed that MoSx was successfully deposited on and was in good contact with the GCNT support. Other physical characterization techniques suggested the amorphous nature of the deposited MoSx. With a typical catalyst loading of 3 mg cm(-2), an overpotential of 141 mV was required to obtain a current density of 10 mA cm(-2). A Tafel slope of 41 mV decade(-1) was demonstrated. Both measures placed the MoSx-deposited GCNT electrode among the best performing molybdenum sulfide-based HER catalysts reported to date. The electrode showed a good stability with only a 25 mV increase in overpotential required for a current density of 10 mA cm(-2), after undergoing 500 potential sweeps with vigorous bubbling present. The current density obtained at -0.5 V vs SHE (Standard Hydrogen Electrode potential) decreased less than 10% after the stability test. The deposition of MoSx on high specific surface area conductive electrodes demonstrated to be an efficient method to maximize the catalytic performance toward HER. PMID:26864503

  7. Novel growth method of carbon nanotubes using catalyst-support layer developed by alumina grit blasting

    Science.gov (United States)

    Watanabe, Hiromichi; Ishii, Juntaro; Ota, Keishin

    2016-08-01

    We propose an efficient method of growing carbon nanotube (CNT) arrays on a variety of metals, alloys, and carbon materials using chemical vapor deposition (CVD) assisted by a simple surface treatment of the materials. The main feature of this method is the application of grit blasting with fine alumina particles to the development of a catalyst-support layer required for the growth of CNTs on various conductive materials, including ultra-hard metals such as tungsten. Auger electron spectroscopy shows that grit blasting can form a non-continuous layer where alumina nanoparticles are embedded as residues in the blasting media left on the treated surfaces. This work reveals that such a non-continuous alumina layer can behave as the catalyst-support layer, which is generally prepared by sputter or a vacuum evaporation coating process that considerably restricts the practical applications of CNTs. We have attempted to grow CNTs on grit-blasted substrates of eighteen conventionally used conductive materials using CVD together with a floating iron catalyst. The proposed method was successful in growing multi-walled CNT arrays on the grit-blasted surfaces of all the examined materials, demonstrating its versatility. Furthermore, we found that the group IV metal oxide films thermally grown on the as-received substrates can support the catalytic activity of iron nanoparticles in the CVD process just as well as the alumina film developed by grit blasting. Spectral emissivity of the CNT arrays in the visible and infrared wavelength ranges has been determined to assess the applicability of the CNT arrays as a black coating media.

  8. Metal Doping Effect of the M-Co2P/Nitrogen-Doped Carbon Nanotubes (M = Fe, Ni, Cu) Hydrogen Evolution Hybrid Catalysts.

    Science.gov (United States)

    Pan, Yuan; Liu, Yunqi; Lin, Yan; Liu, Chenguang

    2016-06-01

    The enhancement of catalytic performance of cobalt phosphide-based catalysts for the hydrogen evolution reaction (HER) is still challenging. In this work, the doping effect of some transition metal (M = Fe, Ni, Cu) on the electrocatalytic performance of the M-Co2P/NCNTs (NCNTs, nitrogen-doped carbon nanotubes) hybrid catalysts for the HER was studied systematically. The M-Co2P/NCNTs hybrid catalysts were synthesized via a simple in situ thermal decomposition process. A series of techniques, including X-ray diffraction, X-ray photoelectron spectroscopy, inductively coupled plasma-optical emission spectrometry, transmission electron microscopy, and N2 sorption were used to characterize the as-synthesized M-Co2P/NCNTs hybrid catalysts. Electrochemical measurements showed the catalytic performance according to the following order of Fe-Co2P/NCNTs > Ni-Co2P/NCNTs > Cu-Co2P/NCNTs, which can be ascribed to the difference of structure, morphology, and electronic property after doping. The doping of Fe atoms promote the growth of the [111] crystal plane, resulting in a large specific area and exposing more catalytic active sites. Meanwhile, the Fe(δ+) has the highest positive charge among all the M-Co2P/NCNTs hybrid catalysts after doping. All these changes can be used to contribute the highest electrocatalytic activity of the Fe-Co2P/NCNTs hybrid catalyst for HER. Furthermore, an optimal HER electrocatalytic activity was obtained by adjusting the doping ratio of Fe atoms. Our current research indicates that the doping of metal is also an important strategy to improve the electrocatalytic activity for the HER. PMID:27197546

  9. Multiwalled Carbon Nanotube Forest Grown via Chemical Vapor Deposition from Iron Catalyst Nanoparticles, by XPS

    Energy Technology Data Exchange (ETDEWEB)

    Jensen, David S.; Kanyal, Supriya S.; Madaan, Nitesh; Vail, Michael A.; Dadson, Andrew; Engelhard, Mark H.; Linford, Matthew R.

    2013-09-25

    Carbon nanotubes (CNTs) have unique chemical and physical properties. Herein, we report an XPS analysis of a forest of multiwalled CNTs using monochromatic Al Kα radiation. Survey scans show only one element: carbon. The carbon 1s peak is centered 284.5 eV. The C 1s envelope also shows the expected π → π* shake-up peak at ca. 291 eV. The valence band and carbon KVV Auger signals are presented. When patterned, the CNT forests can be used as a template for subsequent deposition of metal oxides to make thin layer chromatography plates.1-3

  10. Carbon nanotubes on carbon fibers: Synthesis, structures and properties

    Science.gov (United States)

    Zhang, Qiuhong

    The interface between carbon fibers (CFs) and the resin matrix in traditional high performance composites is characterized by a large discontinuity in mechanical, electrical, and thermal properties which can cause inefficient energy transfer. Due to the exceptional properties of carbon nanotubes (CNTs), their growth at the surface of carbon fibers is a promising approach to controlling interfacial interactions and achieving the enhanced bulk properties. However, the reactive conditions used to grow carbon nanotubes also have the potential to introduce defects that can degrade the mechanical properties of the carbon fiber (CF) substrate. In this study, using thermal chemical vapor deposition (CVD) method, high density multi-wall carbon nanotubes have been successfully synthesized directly on PAN-based CF surface without significantly compromising tensile properties. The influence of CVD growth conditions on the single CF tensile properties and carbon nanotube (CNT) morphology was investigated. The experimental results revealed that under high temperature growth conditions, the tensile strength of CF was greatly decreased at the beginning of CNT growth process with the largest decrease observed for sized CFs. However, the tensile strength of unsized CFs with CNT was approximately the same as the initial CF at lower growth temperature. The interfacial shear strength of CNT coated CF (CNT/CF) in epoxy was studied by means of the single-fiber fragmentation test. Results of the test indicate an improvement in interfacial shear strength with the addition of a CNT coating. This improvement can most likely be attributed to an increase in the interphase yield strength as well as an improvement in interfacial adhesion due to the presence of the nanotubes. CNT/CF also offers promise as stress and strain sensors in CF reinforced composite materials. This study investigates fundamental mechanical and electrical properties of CNT/CF using nanoindentation method by designed

  11. In-situ Measurements of the Effect of Au Doping in Ni Catalysts on the Yield of Tubular Carbon Nanostructures

    DEFF Research Database (Denmark)

    Sharma, Renu; Chee, S.; Rez, P.;

    . Here we show that the yield of tubular carbon structures can be increased by doping a Ni catalyst with Au, and that their morphology and structure can be controlled by varying the reaction temperature. However, the exact role of Au for catalysis is not well understood. Au/Ni thin films (1-2 nm...... with herring-bone, stacked rings and multiwalled structure were observed to form depending upon the reaction temperature and pressure. Atomic resolution videos reveal that the graphene layers (the essential topological form of carbon for tubular growth) form at facets of the crystalline catalyst particles...

  12. Preparation of Co-Mo catalyst using activated carbon produced from egg shell and SiO2 as support – A hydrogenation study

    Directory of Open Access Journals (Sweden)

    Adeniyi Sunday Ogunlaja

    2010-12-01

    Full Text Available The preparation of a series of cobalt-molybdenum (Co-Mo catalysts supported on SiO2 and carbonized egg shells were investigated using standard procedures; the catalysts were further calcined at the 500 oC temperature to generate the internally consistent set, and the metal atoms content were varied in a regular manner. The ratio 1:4 (Co2+: Mo6+ by weight was employed for the various catalysts prepared. The carbonized egg shells were divided into two parts: the first part was leached with HNO3, as the other one was not leached. Activity tests were run using these catalysts containing leached and unleached carbon for the hydrogenation of methyl orange; the changes in absorbance regarding the unhydrogenated methyl orange at a wavelength of 460 nm were respectively 0.07 and 0.067 when the catalyst containing the leached carbonized egg shell (catalyst A and the catalyst containing the unleached activated carbon (catalyst B were used for the hydrogenation reaction. This confirms that catalyst A is more efficient in hydrogenating methyl orange than catalyst B.

  13. Beneficial effects of rhodium and tin oxide on carbon supported platinum catalysts for ethanol electrooxidation

    Science.gov (United States)

    Soares, Layciane A.; Morais, Claudia; Napporn, Teko W.; Kokoh, K. Boniface; Olivi, Paulo

    2016-05-01

    This work investigates ethanol electrooxidation on Pt/C, PtxRhy/C, Pt-SnO2/C, and PtxRhy-SnO2/C catalysts synthesized by the Pechini and microwave-assisted polyol methods. The catalysts are characterized by energy dispersive X-ray analysis (EDX), transmission electron microscopy (TEM), and X-ray diffraction (XRD) techniques. The electrochemical properties of these electrode materials are examined by cyclic voltammetry and chronoamperometry experiments in acid medium. The products obtained during ethanol electrolysis are identified by high performance liquid chromatography (HPLC). The adsorbed intermediates are evaluated by an in situ reflectance Infrared Spectroscopy technique combined with cyclic voltammetry. Catalysts performance in a direct ethanol fuel cell (DEFC) is also assessed. The electrical performance of the electrocatalysts in a single DEFC at 80 °C decreases in the following order Pt70Rh30SnO2 > Pt80Rh20SnO2 > Pt60Rh40SnO2 ∼ PtSnO2 > PtxRhy ∼ Pt, showing that the presence of SnO2 enhances the ability of Pt to catalyze ethanol electrooxidation.

  14. Adsorption and Deactivation Characteristics of Cu/ZnO-Based Catalysts for Methanol Synthesis from Carbon Dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Natesakhawat, Sittichai; Ohodnicki, Paul R; Howard, Bret H; Lekse, Jonathan W; Baltrus, John P; Matranga, Christopher

    2013-07-09

    The adsorption and deactivation characteristics of coprecipitated Cu/ZnO-based catalysts were examined and correlated to their performance in methanol synthesis from CO₂ hydrogenation. The addition of Ga₂O₃ and Y₂O₃ promoters is shown to increase the Cu surface area and CO₂/H₂ adsorption capacities of the catalysts and enhance methanol synthesis activity. Infrared studies showed that CO₂ adsorbs spontaneously on these catalysts at room temperature as both monoand bi-dentate carbonate species. These weakly bound species desorb completely from the catalyst surface by 200 °C while other carbonate species persist up to 500 °C. Characterization using N₂O decomposition, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM) with energy-dispersive X-ray spectroscopy (EDX) analysis clearly indicated that Cu sintering is the main cause of catalyst deactivation. Ga and Y promotion improves the catalyst stability by suppressing the agglomeration of Cu and ZnO particles under pretreatment and reaction conditions.

  15. Nanostructured composite TiO{sub 2}/carbon catalysts of high activity for dehydration of n-butanol

    Energy Technology Data Exchange (ETDEWEB)

    Cyganiuk, Aleksandra [Faculty of Chemistry, Nicolaus Copernicus University, 87-100 Torun (Poland); Klimkiewicz, Roman [Institute of Low Temperature and Structure Research PAN, 50-422 Wroclaw (Poland); Bumajdad, Ali [Faculty of Science, Kuwait University, PO Box 5969 Safat, Kuwait 13060 (Kuwait); Ilnicka, Anna [Faculty of Chemistry, Nicolaus Copernicus University, 87-100 Torun (Poland); Lukaszewicz, Jerzy P., E-mail: jerzy_lukaszewicz@o2.pl [Faculty of Chemistry, Nicolaus Copernicus University, 87-100 Torun (Poland)

    2015-08-15

    Highlights: • New biotechnological method for fabrication of composite catalysts. • In situ synthesis of nanosized TiO{sub 2} clusters in the carbon matrix. • High dispersion of TiO{sub 2} in carbon matrix. • High catalytic activity achieved for very low active phase content. • Efficient dehydration of n-butanol to butane-1. - Abstract: A novel method of wood impregnation with titanium ions is presented. Titanium(IV) ions were complexed to peroxo/hydroxo complexes which were obtained by treating a TiCl{sub 4} water solution with H{sub 2}O{sub 2}. The solution of chelated titanium ions was used for the impregnation of living stems of Salix viminalis wood. Saturated stems were carbonized at 600–800 °C, yielding a microporous carbon matrix, in which nanoparticles of TiO{sub 2} were uniformly distributed. A series of composite TiO{sub 2}–carbon catalysts was manufactured and tested in the process of n-butanol conversion to butane-1. The composite catalysts exhibited very high selectivity (ca. 80%) and yield (ca. 30%) despite a low content of titanium (ca. 0.5% atomic). The research proved that the proposed functionalization led to high dispersion of the catalytic phase (TiO{sub 2}), which played a crucial role in the catalyst performance. High dispersion of TiO{sub 2} was achieved due to a natural transport of complexed titanium ions in living plant stems.

  16. A palladium-doped ceria@carbon core-sheath nanowire network: a promising catalyst support for alcohol electrooxidation reactions

    Science.gov (United States)

    Tan, Qiang; Du, Chunyu; Sun, Yongrong; Du, Lei; Yin, Geping; Gao, Yunzhi

    2015-08-01

    A novel palladium-doped ceria and carbon core-sheath nanowire network (Pd-CeO2@C CSNWN) is synthesized by a template-free and surfactant-free solvothermal process, followed by high temperature carbonization. This hierarchical network serves as a new class of catalyst support to enhance the activity and durability of noble metal catalysts for alcohol oxidation reactions. Its supported Pd nanoparticles, Pd/(Pd-CeO2@C CSNWN), exhibit >9 fold increase in activity toward the ethanol oxidation over the state-of-the-art Pd/C catalyst, which is the highest among the reported Pd systems. Moreover, stability tests show a virtually unchanged activity after 1000 cycles. The high activity is mainly attributed to the superior oxygen-species releasing capability of Pd-doped CeO2 nanowires by accelerating the removal of the poisoning intermediate. The unique interconnected one-dimensional core-sheath structure is revealed to facilitate immobilization of the metal catalysts, leading to the improved durability. This core-sheath nanowire network opens up a new strategy for catalyst performance optimization for next-generation fuel cells.A novel palladium-doped ceria and carbon core-sheath nanowire network (Pd-CeO2@C CSNWN) is synthesized by a template-free and surfactant-free solvothermal process, followed by high temperature carbonization. This hierarchical network serves as a new class of catalyst support to enhance the activity and durability of noble metal catalysts for alcohol oxidation reactions. Its supported Pd nanoparticles, Pd/(Pd-CeO2@C CSNWN), exhibit >9 fold increase in activity toward the ethanol oxidation over the state-of-the-art Pd/C catalyst, which is the highest among the reported Pd systems. Moreover, stability tests show a virtually unchanged activity after 1000 cycles. The high activity is mainly attributed to the superior oxygen-species releasing capability of Pd-doped CeO2 nanowires by accelerating the removal of the poisoning intermediate. The unique

  17. Chemical and toxicological properties of emissions from CNG transit buses equipped with three-way catalysts compared to lean-burn engines and oxidation catalyst technologies

    Science.gov (United States)

    Yoon, Seungju; Hu, Shaohua; Kado, Norman Y.; Thiruvengadam, Arvind; Collins, John F.; Gautam, Mridul; Herner, Jorn D.; Ayala, Alberto

    2014-02-01

    Chemical and toxicological properties of emissions from compressed natural gas (CNG) fueled transit buses with stoichiometric combustion engines and three-way catalyst (TWC) exhaust control systems were measured using a chassis dynamometer testing facility and compared to the data from earlier CNG engine and exhaust control technologies. Gaseous and particulate matter emissions from buses with stoichiometric engines and TWC were significantly lower than the emissions from buses with lean-burn engines. Carbonyls and volatile organic compounds (VOCs) from buses with stoichiometric engines and TWC were lower by more than 99% compared to buses with lean-burn engines. Elemental and organic carbons (EC and OC), polycyclic aromatic hydrocarbons (PAHs), and trace elements from buses with stoichiometric engines and TWC were effectively controlled and significantly lower than the emissions from buses with lean-burn engines. Potential mutagenicity measured using a microsuspension modification of the Salmonella/microsome assay was lower by more than 99% for buses with stoichiometric engines and TWC, compared to buses with lean-burn engines and OxC.

  18. Catalytic Chemical Vapor Deposition of Methane to Carbon Nanotubes: Copper Promoted Effect of Ni/MgO Catalysts

    Directory of Open Access Journals (Sweden)

    Wen Yang

    2014-01-01

    Full Text Available The Ni/MgO and Ni-Cu/MgO catalysts were prepared by sol-gel method and used as the catalysts for synthesis of carbon nanotubes by thermal chemical vapor deposition. The effect of Cu on the carbon yield and structure was investigated, and the effects of calcination temperature and reaction temperature were also investigated. The catalysts and synthesized carbon materials were characterized by temperature programmed reduction (TPR, thermogravimetric analysis (TGA, and scanning electron microscopy (SEM. Results showed that the addition of Cu promoted the reduction of nickel species, subsequently improving the growth and yield of CNTs. Meanwhile, CNTs were synthesized by the Ni/MgO and Ni-Cu/MgO catalysts with various calcination temperatures and reaction temperatures, and results suggested that the obtained CNTs on Ni-Cu/MgO catalyst with the calcination temperature of 500°C and the reaction temperature of 650°C were of the greatest yield and quantity of 927%.

  19. Direct observation of morphological evolution of a catalyst during carbon nanotube forest growth: new insights into growth and growth termination

    Science.gov (United States)

    Jeong, Seojeong; Lee, Jaegeun; Kim, Hwan-Chul; Hwang, Jun Yeon; Ku, Bon-Cheol; Zakharov, Dmitri N.; Maruyama, Benji; Stach, Eric A.; Kim, Seung Min

    2016-01-01

    In this study, we develop a new methodology for transmission electron microscopy (TEM) analysis that enables us to directly investigate the interface between carbon nanotube (CNT) arrays and the catalyst and support layers for CNT forest growth without any damage induced by a post-growth TEM sample preparation. Using this methodology, we perform in situ and ex situ TEM investigations on the evolution of the morphology of the catalyst particles and observe the catalyst particles to climb up through CNT arrays during CNT forest growth. We speculate that the lifted catalysts significantly affect the growth and growth termination of CNT forests along with Ostwald ripening and sub-surface diffusion. Thus, we propose a modified growth termination model which better explains various phenomena related to the growth and growth termination of CNT forests.In this study, we develop a new methodology for transmission electron microscopy (TEM) analysis that enables us to directly investigate the interface between carbon nanotube (CNT) arrays and the catalyst and support layers for CNT forest growth without any damage induced by a post-growth TEM sample preparation. Using this methodology, we perform in situ and ex situ TEM investigations on the evolution of the morphology of the catalyst particles and observe the catalyst particles to climb up through CNT arrays during CNT forest growth. We speculate that the lifted catalysts significantly affect the growth and growth termination of CNT forests along with Ostwald ripening and sub-surface diffusion. Thus, we propose a modified growth termination model which better explains various phenomena related to the growth and growth termination of CNT forests. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr05547d

  20. An in-depth understanding of the bimetallic effects and coked carbon species on an active bimetallic Ni(Co)/Al2O3 dry reforming catalyst.

    Science.gov (United States)

    Liao, Xin; Gerdts, Rihards; Parker, Stewart F; Chi, Lina; Zhao, Yongxiang; Hill, Martyn; Guo, Junqiu; Jones, Martin O; Jiang, Zheng

    2016-06-29

    Ni/Al2O3, Co/Al2O3 and bimetallic Ni(Co)/Al2O3 catalysts were prepared using an impregnation method and employed in CO2 dry reforming of methane under coking-favored conditions. The spent catalysts were carefully characterized using typical characterization technologies and inelastic neutron scattering spectroscopy. The bimetallic catalyst exhibited a superior activity and anti-coking performance compared to Ni/Al2O3, while the most resistant to coking behavior was Co/Al2O3. The enhanced activity of the Ni(Co)/Al2O3 bimetallic catalyst is attributed to the reduced particle size of metallic species and resistance to forming stable filamentous carbon. The overall carbon deposition on the spent bimetallic catalyst is comparable to that of the spent Ni/Al2O3 catalyst, whereas the carbon deposited on the bimetallic catalyst is mainly less-stable carbonaceous species as confirmed by SEM, TPO, Raman and INS characterization. This study provides an in depth understanding of alloy effects in catalysts, the chemical nature of coked carbon on spent Ni-based catalysts and, hopefully, inspires the creative design of a new bimetallic catalyst for dry reforming reactions.

  1. Multi-Walled Carbon Nanotubes as a Catalyst for Gas-Phase Oxidation of Ethanol to Acetaldehyde.

    Science.gov (United States)

    Wang, Jia; Huang, Rui; Feng, Zhenbao; Liu, Hongyang; Su, Dangsheng

    2016-07-21

    Multi-walled carbon nanotubes (CNTs) were directly used as a sustainable and green catalyst to convert ethanol into acetaldehyde in the presence of molecular oxygen. The C=O groups generated on the nanocarbon surface were demonstrated as active sites for the selective oxidation of ethanol to acetaldehyde. The transformation of disordered carbon debris on the CNT surface to ordered graphitic structures induced by thermal-treatment significantly enhanced the stability of the active C=O groups, and thus the catalytic performance. A high reactivity with approximately 60 % ethanol conversion and 93 % acetaldehyde selectivity was obtained over the optimized CNT catalyst at 270 °C. More importantly, the catalytic performance was quite stable even after 500 h, which is comparable with a supported gold catalyst. The robust catalytic performance displayed the potential application of CNTs in the industrial catalysis field. PMID:27282126

  2. Low-temperature growth of nitrogen-doped carbon nanofibers by acetonitrile catalytic CVD using Ni-based catalysts

    Science.gov (United States)

    Iwasaki, Tomohiro; Makino, Yuri; Fukukawa, Makoto; Nakamura, Hideya; Watano, Satoru

    2016-06-01

    To synthesize nitrogen-doped carbon nanofibers (N-CNFs) at high growth rates and low temperatures less than 673 K, nickel species (metallic nickel and nickel oxide) supported on alumina particles were used as the catalysts for an acetonitrile catalytic chemical vapor deposition (CVD) process. The nickel:alumina mass ratio in the catalysts was fixed at 0.05:1. The catalyst precursors were prepared from various nickel salts (nitrate, chloride, sulfate, acetate, and lactate) and then calcined at 1073 K for 1 h in oxidative (air), reductive (hydrogen-containing argon), or inert (pure argon) atmospheres to activate the nickel-based catalysts. The effects of precursors and calcination atmosphere on the catalyst activity at low temperatures were studied. We found that the catalysts derived from nickel nitrate had relatively small crystallite sizes of nickel species and provided N-CNFs at high growth rates of 57 ± 4 g-CNF/g-Ni/h at 673 K in the CVD process using 10 vol% hydrogen-containing argon as the carrier gas of acetonitrile vapor, which were approximately 4 times larger than that of a conventional CVD process. The obtained results reveal that nitrate ions in the catalyst precursor and hydrogen in the carrier gas can contribute effectively to the activation of catalysts in low-temperature CVD. The fiber diameter and nitrogen content of N-CNFs synthesized at high growth rates were several tens of nanometers and 3.5 ± 0.3 at.%, respectively. Our catalysts and CVD process may lead to cost reductions in the production of N-CNFs.

  3. Super-hydrophobic transparent surface by femtosecond laser micro-patterned catalyst thin film for carbon nanotube cluster growth

    Science.gov (United States)

    Tang, M.; Hong, M. H.; Choo, Y. S.; Tang, Z.; Chua, Daniel H. C.

    2010-11-01

    In this work, super-hydrophobic surfaces were fabricated by femtosecond laser micro-machining and chemical vapor deposition to constitute hybrid scale micro/nano-structures formed by carbon nanotube (CNT) clusters. Nickel thin-film microstructures, functioning as CNT growth catalyst, precisely control the distribution of the CNT clusters. To obtain minimal heat-affected zones, femtosecond laser was used to trim the nickel thin-film coating. Plasma treatment was subsequently carried out to enhance the lotus-leaf effect. The wetting property of the CNT surface is improved from hydrophilicity to super-hydrophobicity at an advancing contact angle of 161 degrees. The dynamic water drop impacting test further confirms its enhanced water-repellent property. Meanwhile, this super-hydrophobic surface exhibits excellent transparency with quartz as the substrate. This hybrid fabrication technique can achieve super-hydrophobic surfaces over a large area, which has potential applications as self-cleaning windows for vehicles, solar cells and high-rise buildings.

  4. Synthesis and Electrochemical Properties of Carbon Nanofibers and SiO2/Carbon Nanofiber Composite on Ni-Cu/C-Fiber Textiles.

    Science.gov (United States)

    Nam, Ki-Mok; Park, Heai-Ku; Lee, Chang-Seop

    2015-11-01

    In this study, carbon nanofibers (CNFs) were grown by chemical vapor deposition on C-fiber textiles that had Ni and Cu catalyst deposited via electrophoretic deposition. Before the CNFs were coated with silica layer via hydrolysis of TEOS (Tetraethyl orthosilicate), the carbon nanofibers were oxidized by nitric acid. Due to oxidation, the hydroxyl group was created on the carbon nanofibers and this was used as an activation site for the SiO2. The physicochemical properties of the grown carbon nanofibers were investigated with Scanning electron microscopy (SEM), Energy dispersive spectroscopy (EDS), X-ray Diffraction (XRD), Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS). The structures of SiO2-coated carbon nanofibers were characterized by XPS and TEM. The electrochemical properties and the capacitance of the materials were investigated by galvanostatic charge-discharge and cyclic voltammetry. Different types of carbon nanofibers were grown upon the deposition utilizing catalysts, with the SiO2 uniformly coated on the surface of carbon nanofibers. When used as an anode material for the Li secondary battery, the SiO2/CNFs composite had a lower capacity maintenance and a greater discharge capacity as compared to the carbon nanofibers.

  5. Multi-walled carbon nanotubes as catalyst promoter for dimethyl ether synthesis from CO{sub 2} hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Zha, Fei, E-mail: zhafei@nwnu.edu.cn [College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070 (China); Tian, Haifeng; Yan, Jun [College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070 (China); Chang, Yue [College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070 (China); Key Laboratory of Polymer Material of Gansu Province, Lanzhou 730070 (China)

    2013-11-15

    The mixed acid of H{sub 2}SO{sub 4}/HNO{sub 3}-pretreated multi-walled carbon nanotubes was employed as supports and ultrasound-assisted co-precipitation method was designed to prepare multi-walled carbon nanotubes supported CuO–ZnO–Al{sub 2}O{sub 3}/HZSM-5 catalyst. The catalyst was characterized by means of X-ray diffraction spectrum (XRD), scanning electron microscope (SEM), transmission electron microscopy (TEM), thermal analysis (TG) and Brunauer–Emmett–Teller (BET). The catalyst activity for the preparation of dimethyl ether from hydrogenation of CO{sub 2} was investigated in a fixed-bed reactor, which showed that multi-walled carbon nanotubes could promote the catalyst activity of CuO–ZnO–Al{sub 2}O{sub 3}/HZSM-5. Under the reaction conditions of temperature at 262 °C, pressure at 3.0 MPa, H{sub 2}/CO{sub 2} = 3 (volume ratio) and space velocity (SV) = 1800 mL g{sub cat}{sup −1} h{sup −1}, the conversion per pass of carbon dioxide was 46.2%, with the dimethyl ether yield and selectivity of 20.9% and 45.2%.

  6. Hydroxyapatite supported caesium carbonate as a new recyclable solid base catalyst for the Knoevenagel condensation in water

    Directory of Open Access Journals (Sweden)

    Monika Gupta

    2009-11-01

    Full Text Available The Knoevenagel condensation between aromatic aldehydes and malononitrile, ethyl cyanoacetate or malonic acid with hydroxyapatite supported caesium carbonate in water is described. HAP–Cs2CO3 was found to be a highly active, stable and recyclable catalyst under the reaction conditions.

  7. Hydroxyapatite supported caesium carbonate as a new recyclable solid base catalyst for the Knoevenagel condensation in water

    OpenAIRE

    Monika Gupta; Rajive Gupta; Medha Anand

    2009-01-01

    The Knoevenagel condensation between aromatic aldehydes and malononitrile, ethyl cyanoacetate or malonic acid with hydroxyapatite supported caesium carbonate in water is described. HAP–Cs2CO3 was found to be a highly active, stable and recyclable catalyst under the reaction conditions.

  8. Size and Promoter Effects on Stability of Carbon-Nanofiber-Supported Iron-Based Fischer-Tropsch Catalysts

    NARCIS (Netherlands)

    Xie, Jingxiu; Torres Galvis, Hirsa; Koeken, Ard C J; Kirilin, Alexey; Dugulan, A Iulian; Ruitenbeek, Matthijs; de Jong, Krijn P

    2016-01-01

    The Fischer-Tropsch Synthesis converts synthesis gas from alternative carbon resources, including natural gas, coal, and biomass, to hydrocarbons used as fuels or chemicals. In particular, iron-based catalysts at elevated temperatures favor the selective production of C2-C4 olefins, which are import

  9. Formation of isolated carbon nanofibers with hot-wire CVD using nanosphere lithography as catalyst patterning technique

    NARCIS (Netherlands)

    Houweling, Z.S.; Verlaan, V.; ten Grotenhuis, G.T.; Schropp, R.E.I.

    2008-01-01

    Recently the site-density control of carbon nanotubes (CNTs) has attracted much attention as this has become critical for its many applications. To obtain an ordered array of catalyst nanoparticles with good monodispersity nanosphere lithography (NSL) is used. These nanoparticles are tested as catal

  10. High Throughput Nanofabrication of Silicon Nanowire and Carbon Nanotube Tips on AFM Probes by Stencil-Deposited Catalysts

    DEFF Research Database (Denmark)

    Engstrøm, Daniel Southcott; Savu, Veronica; Zhu, Xueni;

    2011-01-01

    A new and versatile technique for the wafer scale nanofabrication of silicon nanowire (SiNW) and multiwalled carbon nanotube (MWNT) tips on atomic force microscope (AFM) probes is presented. Catalyst material for the SiNW and MWNT growth was deposited on prefabricated AFM probes using aligned wafer...

  11. Three-dimensional shapes and spatial distributions of Pt and PtCr catalyst nanoparticles on carbon black

    DEFF Research Database (Denmark)

    Gontard, Lionel Cervera; Dunin-Borkowski, Rafal E.; Ozkaya, D.

    2008-01-01

    High-angle annular dark-field scanning transmission electron microscopy tomography is applied to the study of Pt and PtCr nanoparticles supported on carbon black, which are used as heterogeneous catalysts in the electrodes of proton exchange membrane fuel cells. By using electron tomography, the...

  12. Microcalorimetric Adsorption of Alumina Oxide Catalysts for Combination of Ethylbenzene dehydrogenation and carbon Dioxide Shift-reaction

    Institute of Scientific and Technical Information of China (English)

    GE Xin; SHEN Jian-yi

    2004-01-01

    Styrene (STY) is now produced industrially in fairly large quantities by the dehydrogenation of ethylbenzene (EB) using promoted iron oxide catalyst with superheated steam.In this case, small amount of carbon dioxide formed as a by-product was known to inhibit the catalytic activity of commercial catalyst. Recently, there have been some reports which carbon dioxide showed positive effects to promote catalytic activities on the reaction over several catalysts.In this study, we attempted to combine the dehydrogenation of EB to STY with the carbon dioxide shift-reaction. The combine reaction (EB + CO2 → STY + H2O + CO) can be considered as one of the ways of using CO2 resources and can yield simultaneously STY and Carbon oxide.Alumina oxide catalysts such as Al2O3, Na2O/Al2O3 and K2O/Al2O3 were prepared by the usual impregnation method with an aqueous solution of NaNO3 and KNO3, and then calcined at 650℃ for 5 h in a stream of air. The reaction condition is 600℃, flow of CO2 38ml/mon and space velocity (EB) 1.28h-1.

  13. N-Co-O Triply Doped Highly Crystalline Porous Carbon: An Acid-Proof Nonprecious Metal Oxygen Evolution Catalyst.

    Science.gov (United States)

    Yang, Shiliu; Zhan, Yi; Li, Jingfa; Lee, Jim Yang

    2016-02-10

    In comparison with nonaqueous Li-air batteries, aqueous Li-air batteries are kinetically more facile and there is more variety of non-noble metal catalysts available for oxygen electrocatalysis, especially in alkaline solution. The alkaline battery environment is however vulnerable to electrolyte carbonation by atmospheric CO2 resulting in capacity loss over time. The acid aqueous solution is immune to carbonation but is limited by the lack of effective non-noble metal catalysts for the oxygen evolution reaction (OER). This is contrary to the oxygen reduction reaction (ORR) in acid solution where a few good candidates exist. We report here the development of a N-Co-O triply doped carbon catalyst with substantial OER activity in acid solution by the thermal codecomposition of polyaniline, cobalt salt and cyanamide in nitrogen. Cyanamide and the type of cobalt precursor salt were found to determine the structure, crystallinity, surface area, extent of Co doping and consequently the OER activity of the final carbon catalyst in acid solution. We have also put forward some hypotheses about the active sites that may be useful for guiding further work. PMID:26795393

  14. Developing an approach for first-principles catalyst design: application to carbon-capture catalysis.

    Science.gov (United States)

    Kulik, Heather J; Wong, Sergio E; Baker, Sarah E; Valdez, Carlos A; Satcher, Joe H; Aines, Roger D; Lightstone, Felice C

    2014-02-01

    An approach to catalyst design is presented in which local potential energy surface models are first built to elucidate design principles and then used to identify larger scaffold motifs that match the target geometries. Carbon sequestration via hydration is used as the model reaction, and three- and four-coordinate sp(2) or sp(3) nitrogen-ligand motifs are considered for Zn(II) metals. The comparison of binding, activation and product release energies over a large range of interaction distances and angles suggests that four-coordinate short Zn(II)-Nsp(3) bond distances favor a rapid turnover for CO2 hydration. This design strategy is then confirmed by computationally characterizing the reactivity of a known mimic over a range of metal-nitrogen bond lengths. A search of existing catalysts in a chemical database reveals structures that match the target geometry from model calculations, and subsequent calculations have identified these structures as potentially effective for CO2 hydration and sequestration. PMID:24508957

  15. Platinum supported catalysts for carbon monoxide preferential oxidation: Study of support influence

    Energy Technology Data Exchange (ETDEWEB)

    Padilla, R.; Rodriguez, L.; Serrano-Lotina, A.; Daza, L. [Instituto de Catalisis y Petroleoquimica (CSIC), C/Marie Curie 2, Campus Cantoblanco, 28049 Madrid (Spain); Benito, M. [Instituto de Catalisis y Petroleoquimica (CSIC), C/Marie Curie 2, Campus Cantoblanco, 28049 Madrid (Spain); Centro de Investigaciones Energeticas Medioambientales y Tecnologicas (CIEMAT), Av. Complutense 22, 28040 Madrid (Spain)

    2009-07-01

    The aim of this work is to study the influence of the addition of different oxides to an alumina support, on surface acidity and platinum reducibility in platinum-based catalysts, as well as their effect on the activity and selectivity in CO preferential oxidation, in presence of hydrogen. A correlation between surface acidity and acid strength of surface sites and metal reducibility was obtained, being Pt-support interaction a function of the acid sites concentration under a particular temperature range. In platinum supported on alumina catalysts, CO oxidation follows a Langmuir-Hinshelwood mechanism, where O{sub 2} and CO compete in the adsorption on the same type of active sites. It is noteworthy that the addition of La{sub 2}O{sub 3} modifies the reaction mechanism. In this case, CO is not only adsorbed on the Pt active sites but also on La{sub 2}O{sub 3}, forming bridge bonded carbonates which leads to high reactivity at low temperatures. An increase on temperature produces CO desorption from Pt surface sites and favours oxygen adsorption producing CO{sub 2}. CO oxidation with surface hydroxyl groups was activated producing simultaneously CO{sub 2} and H{sub 2}. (author)

  16. Preparation and characterization of hydrophobic platinum-doped carbon aerogel catalyst for hydrogen isotope separation

    Indian Academy of Sciences (India)

    M K Singh; R Singh; A Singh; D K Kohli; U Deshpande; P K Gupta

    2014-10-01

    We report preparation of hydrophobic platinum-doped carbon aerogel (PtCA) catalyst and its characterization for catalytic exchange reactions between hydrogen isotopes. The PtCA powder was synthesized by sol–gel polymerization method, mixed with colloidal PTFE solution, and coated on Dixon rings to obtain hydrophobic catalyst. The Pt cluster size in PtCA powder was observed to vary from 3 to 5 nm for a change in resorcinol to alkali molar ratio in synthesis solution from 20 to 200. Transmission electron microscopy of powder showed that the Pt clusters were uniformally dispersed and Pt0 metallic content estimated by X-ray photoelectron spectroscopy (XPS) was found to be of ∼ 70%. The catalytic activity was found to depend on Pt cluster size and was higher for smaller cluster size. For the smallest achieved Pt cluster size of 3 nm, catalytic activity of ∼ 0.8 m3 (STP) s-1 m-3 was obtained for hydrogen isotope exchange in atmospheric pressure conditions.

  17. Developing an approach for first-principles catalyst design: application to carbon-capture catalysis.

    Science.gov (United States)

    Kulik, Heather J; Wong, Sergio E; Baker, Sarah E; Valdez, Carlos A; Satcher, Joe H; Aines, Roger D; Lightstone, Felice C

    2014-02-01

    An approach to catalyst design is presented in which local potential energy surface models are first built to elucidate design principles and then used to identify larger scaffold motifs that match the target geometries. Carbon sequestration via hydration is used as the model reaction, and three- and four-coordinate sp(2) or sp(3) nitrogen-ligand motifs are considered for Zn(II) metals. The comparison of binding, activation and product release energies over a large range of interaction distances and angles suggests that four-coordinate short Zn(II)-Nsp(3) bond distances favor a rapid turnover for CO2 hydration. This design strategy is then confirmed by computationally characterizing the reactivity of a known mimic over a range of metal-nitrogen bond lengths. A search of existing catalysts in a chemical database reveals structures that match the target geometry from model calculations, and subsequent calculations have identified these structures as potentially effective for CO2 hydration and sequestration.

  18. Hydrogenation of Anthracene in Supercritical Carbon Dioxide Solvent Using Ni Supported on Hβ-Zeolite Catalyst

    Directory of Open Access Journals (Sweden)

    Ashraf Aly Hassan

    2012-01-01

    Full Text Available Catalytic hydrogenation of anthracene was studied over Ni supported on Hβ-zeolite catalyst under supercritical carbon dioxide (sc-CO2 solvent. Hydrogenation of anthracene in sc-CO2 yielded 100% conversion at 100 °C, which is attributed to the reduced mass transfer limitations, and increased solubility of H2 and substrate in the reaction medium. The total pressure of 7 MPa was found to be optimum for high selectivity of octahydroanthracene (OHA. The conversion and selectivity for OHA increased with an increase in H2 partial pressure, which is attributed to higher concentration of hydrogen atoms at higher H2 pressures. The selectivity reduced the pressure below 7 MPa because of enhanced desorption of the tetrahydro-molecules and intermediates from Ni active sites, due to higher solubility of the surface species in sc-CO2. The selectivity of OHA increased with the increase in catalyst weight and reaction time. The rate of hydrogenation of anthracene was compared with that found for napthalene and phenanthrene. The use of acetonitrile as co-solvent or expanded liquid with CO2 decreased the catalytic activity.

  19. 利用杂原子调控纳米碳材料催化剂催化能力的初步探索%Computational exploration on effects of heteroatom doping for nanostructured carbon catalysts

    Institute of Scientific and Technical Information of China (English)

    李波; 苏党生

    2014-01-01

    Nanostructured carbon materials have become an important class of non-metal catalysts. One of the effective ways to tailor the properties of nanostructured carbon catalysts is heteroatoms doping. In the current study, three cases were selected to demonstrate the effects of heteroatoms doping with boron or nitrogen. They were partial oxidation of methane, selectivity in oxidative dehydrogenation reaction, and halogenation of acetylene. Computational studies revealed that doping did enhance the catalytic capabilities of nanostructured carbon catalysts. Moreover it could modulate the electronic structure and acid/base properties of the catalysts. The reaction mechanism was different from metal catalyst. Overall, the current study is crucial for the further development of nanostructured carbon catalysts and sheds light on the new strategy for optimization of catalytic performance.%纳米碳材料已经成为一类重要的非金属催化剂。通过在纳米碳材料催化剂中引入杂原子可以有效地改变催化剂的性能。通过3个研究实例分别说明了杂原子硼和氮在甲烷部分氧化、氧化脱氢反应中乙烯选择性和乙炔卤化反应中的作用和机理。通过研究表明硼和氮杂原子可以优化纳米碳材料的催化效果,改变催化剂的电子结构和酸碱性,揭示了碳材料与金属催化剂的不同作用机理。当前计算结果可为进一步提高纳米碳材料催化剂催化能力奠定基础。

  20. Tungsten carbide modified high surface area carbon as fuel cell catalyst support

    Science.gov (United States)

    Shao, Minhua; Merzougui, Belabbes; Shoemaker, Krista; Stolar, Laura; Protsailo, Lesia; Mellinger, Zachary J.; Hsu, Irene J.; Chen, Jingguang G.

    Phase pure WC nanoparticles were synthesized on high surface area carbon black (800 m 2 g -1) by a temperature programmed reaction (TPR) method. The particle size of WC can be controlled under 30 nm with a relatively high coverage on the carbon surface. The electrochemical testing results demonstrated that the corrosion resistance of carbon black was improved by 2-fold with a surface modification by phase pure WC particles. However, the WC itself showed some dissolution under potential cycling. Based on the X-ray diffraction (XRD) and inductively coupled plasma (ICP) analysis, most of the WC on the surface was lost or transformed to oxides after 5000 potential cycles in the potential range of 0.65-1.2 V. The Pt catalyst supported on WC/C showed a slightly better ORR activity than that of Pt/C, with the Pt activity loss rate for Pt/WC/C being slightly slower compared to that of Pt/C. The performance and decay rate of Pt/WC/C were also evaluated in a fuel cell.

  1. High-Yield Synthesis of Helical Carbon Nanofibers Using Iron Oxide Fine Powder as a Catalyst

    Directory of Open Access Journals (Sweden)

    Yoshiyuki Suda

    2015-01-01

    Full Text Available Carbon nanocoil (CNC, which is synthesized by a catalytic chemical vapor deposition (CCVD method, has a coil diameter of 300–900 nm and a length of several tens of μm. Although it is very small, CNC is predicted to have a high mechanical strength and hence is expected to have a use in nanodevices such as electromagnetic wave absorbers and field emitters. For nanodevice applications, it is necessary to synthesize CNC in high yield and purity. In this study, we improved the conditions of catalytic layer formation and CCVD. Using optimized CVD conditions, a CNC layer with a thickness of >40 μm was grown from a SnO2/Fe2O3/SnO2 catalyst on a substrate, and its purity increased to 81% ± 2%.

  2. Thin catalyst layers based on carbon nanotubes for PEM-fuel cell applications

    Science.gov (United States)

    Bohnenberger, T.; Matovic, J.; Schmid, U.

    2011-06-01

    In this study, two approaches are compared to develop thin, multifunctional films of carbon nanotubes (CNT) which are targeted to serve as a catalyst layer in fuel cells. The first is based on the direct deposition of mixed multi- and single-wall CNTs on metalized silicon wafers, using the metallization as a sacrificial layer to subsequently detach the CNT film from the substrate. It is a less time consuming and a straight forward method compared to the alternative under investigation, the layer-by-layer technique (LbL). The LbL uses bilayers of charged nanotubes to slowly build up a film with an exactly defined thickness. The process is well controlled, but the time constants for deposition of each bilayer are rather high (i.e. about 1 h). With additional annealing steps implemented during film generation this method, however, is regarded advantageous as membranes results with improved mechanical stability and a good homogeneity.

  3. Thermal Properties of Hybrid Carbon Nanotube/Carbon Fiber Polymer

    Science.gov (United States)

    Kang, Jin Ho; Cano, Roberto J.; Luong, Hoa; Ratcliffe, James G.; Grimsley, Brian W.; Siochi, Emilie J.

    2016-01-01

    Carbon fiber reinforced polymer (CFRP) composites possess many advantages for aircraft structures over conventional aluminum alloys: light weight, higher strength- and stiffness-to-weight ratio, and low life-cycle maintenance costs. However, the relatively low thermal and electrical conductivities of CFRP composites are deficient in providing structural safety under certain operational conditions such as lightning strikes. One possible solution to these issues is to interleave carbon nanotube (CNT) sheets between conventional carbon fiber (CF) composite layers. However, the thermal and electrical properties of the orthotropic hybrid CNT/CF composites have not been fully understood. In this study, hybrid CNT/CF polymer composites were fabricated by interleaving layers of CNT sheets with Hexcel (Registered Trademark) IM7/8852 prepreg. The CNT sheets were infused with a 5% solution of a compatible epoxy resin prior to composite fabrication. Orthotropic thermal and electrical conductivities of the hybrid polymer composites were evaluated. The interleaved CNT sheets improved the in-plane thermal conductivity of the hybrid composite laminates by about 400% and the electrical conductivity by about 3 orders of magnitude.

  4. Kinetics of carbon monoxide oxidation over modified supported CuO catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Loc, Luu Cam; Tri, Nguyen; Cuong, Hoang Tien; Thoang, Ho Si [Vietnam Academy of Science and Technology (VAST), Ho Chi Minh City (Viet Nam). Inst. of Chemical Technology; Agafonov, Yu.A.; Gaidai, N.A.; Lapidus, A.L. [Russian Academy of Sciences, Moscow (Russian Federation). N.D. Zelinsky Institute of Organic Chemistry

    2013-11-01

    The following supported on {gamma}-Al{sub 2}O{sub 3} catalysts: 10(wt.)%CuO (CuAl), 10%CuO+10%Cr{sub 2}O{sub 3} (CuCrAl) and 10%CuO+20%CeO{sub 2} (CuCeAl) were under the investigation. Physico-chemical characteristics of the catalysts were determined by the methods of BET, X-ray Diffraction (XRD), and Temperature-Programmed Reduction (TPR). A strong interaction of copper with support in CuAl resulted in the formation of low active copper aluminates. The bi-oxide CuCrAl was more active than CuAl owing to the formation of high catalytically active spinel CuCr{sub 2}O{sub 4}. The fact of very high activity of the sample CuCeAl can be explained by the presence of the catalytically active form of CuO-CeO{sub 2}-Al{sub 2}O{sub 3}. The kinetics of CO total oxidation was studied in a gradientless flow-circulating system at the temperature range between 200 C and 270 C. The values of initial partial pressures of carbon monoxide (P{sup o}{sub CO}), oxygen (P{sup o}{sub O2}), and specially added carbon dioxide (P{sup o}{sub CO{sub 2}}) were varied in ranges (hPa): 10 / 45; 33 / 100, and 0 / 30, respectively. (orig.)

  5. Fabrication and Properties of Carbon-Encapsulated Cobalt Nanoparticles over NaCl by CVD.

    Science.gov (United States)

    Li, Haipeng; Li, Yue; Zhang, Yongguang; Liang, Chunyong; Wang, Hongshui; Li, Baoe; Adair, Desmond; Bakenov, Zhumabay

    2016-12-01

    Carbon-encapsulated cobalt (Co@C) nanoparticles, with a tunable structure, were synthesized by chemical vapor deposition using Co nanoparticles as the catalyst and supported on a water-soluble substrate (sodium chloride), which was easily removed by washing and centrifugation. The influences of growth temperature and time on the structure and magnetic properties of the Co@C nanoparticles were systematically investigated. For different growth temperatures, the magnetic Co nanoparticles were encapsulated by different types of carbon layers, including amorphous carbon layers, graphitic layers, and carbon nanofibers. This inferred a close relationship between the structure of the carbon-encapsulated metal nanoparticles and the growth temperature. At a fixed growth temperature of 400 °C, prolonged growth time caused an increase in thickness of the carbon layers. The magnetic characterization indicated that the magnetic properties of the obtained Co@C nanoparticles depend not only on the graphitization but also on the thickness of the encapsulated carbon layer, which were easily controlled by the growth temperatures and times. Optimization of the synthesis process allowed achieving relatively high coercivity of the synthesized Co@C nanoparticles and enhancement of its ferromagnetic properties, which make this system promising as a magnetic material, particularly for high-density magnetic recording applications. PMID:27677303

  6. Removal performance and mechanism of ibuprofen from water by catalytic ozonation using sludge-corncob activated carbon as catalyst.

    Science.gov (United States)

    Wang, Hongjuan; Zhang, Liqiu; Qi, Fei; Wang, Xue; Li, Lu; Feng, Li

    2014-09-01

    To discover the catalytic activity of sludge-corncob activated carbon in catalytic ozonation of Ibuprofen, the performance of sludge-corncob activated carbon and three selected commercial activated carbons as catalysts in catalytic ozonation was investigated. The observation indicates the degradation rate of Ibuprofen increases significantly in the presence of sludge-corncob activated carbon and the catalytic activity of sludge-corncob activated carbon is much higher than that of the other three commercial activated carbons. Ibuprofen's removal rate follows pseudo-first order kinetics model well. It is also found that the adsorption removal of Ibuprofen by sludge-corncob activated carbon is less than 30% after 40 min. And the removal efficiency of Ibuprofen in the hybrid ozone/sludge-corncob activated carbon system is higher than the sum of sludge-corncob activated carbon adsorption and ozonation alone, which is a supportive evidence for catalytic reaction. In addition, the results of radical scavenger experiments demonstrate that catalytic ozonation of Ibuprofen by sludge-corncob activated carbon follows a hydroxyl radical reaction pathway. During ozonation of Ibuprofen in the presence of activated carbon, ozone could be catalytically decomposed to form hydrogen peroxide, which can promote the formation of hydroxyl radical. The maximum amount of hydrogen peroxide occurs in the presence of sludge-corncob activated carbon, which can explain why sludge-corncob activated carbon has the best catalytic activity among four different activated carbons.

  7. TiN@nitrogen-doped carbon supported Pt nanoparticles as high-performance anode catalyst for methanol electrooxidation

    Science.gov (United States)

    Zhang, Jun; Ma, Li; Gan, Mengyu; Fu, Shenna; Zhao, Yi

    2016-08-01

    In this paper, TiN@nitrogen-doped carbons (NDC) composed of a core-shell structure are successfully prepared through self-assembly and pyrolysis treatment using γ-aminopropyltriethoxysilane as coupling agent, polyaniline as carbon and nitrogen source, respectively. Subsequently, TiN@NDC supporting Pt nanoparticles (Pt/TiN@NDC) are obtained by a microwave-assisted polyol process. The nitrogen-containing functional groups and TiN nanoparticles play a critical role in decreasing the average particle size of Pt and improving the electrocatalytic activity of Pt/TiN@NDC. Transmission electron microscope results reveal that Pt nanoparticles are uniformly dispersed in the TiN@NDC surface with a narrow particle size ranging from 1 to 3 nm in diameter. Moreover, the Pt/TiN@NDC catalyst shows significantly improved catalytic activity and high durability for methanol electrooxidation in comparison with Pt/NDC and commercial Pt/C catalysts, revealed by cyclic voltammetry and chronoamperometry. Strikingly, this novel Pt/TiN@NDC catalyst reveals a better CO tolerance related to Pt/NDC and commercial Pt/C catalysts, which due to the bifunctional mechanism and strong metal-support interaction between Pt and TiN@NDC. In addition, the probable reaction steps for the electrooxidation of CO adspecies on Pt NPs on the basis of the bifunctional mechanism are also proposed. These results indicate that the TiN@NDC is a promising catalyst support for methanol electrooxidation.

  8. Increasing the Tensile Property of Unidirectional Carbon/Carbon Composites by Grafting Carbon Nanotubes onto Carbon Fibers by Electrophoretic Deposition

    Institute of Scientific and Technical Information of China (English)

    Qiang Song; Kezhi Li; Hejun Li; Qiangang Fu

    2013-01-01

    Although in-situ growing carbon nanotubes (CNTs) on carbon fibers could greatly increase the matrix-dominated mechanical properties of carbon/carbon composites (C/Cs),it always decreased the tensile strength of carbon fibers.In this work,CNTs were introduced into unidirectional carbon fiber (CF) preforms by electrophoretic deposition (EPD) and they were used to reinforce C/Cs.Effects of the content of CNTs introduced by EPD on tensile property of unidirectional C/Cs were investigated.Results demonstrated that EPD could be used as a simple and efficient method to fabricate carbon nanotube reinforced C/Cs (CNT-C/Cs) with excellent tensile strength,which pays a meaningful way to maximize the global performance of CNT-C/Cs.

  9. Catalytic decomposition of methane to COx-free hydrogen and carbon nanotubes over Co–W/MgO catalysts

    Directory of Open Access Journals (Sweden)

    Ahmed E. Awadallah

    2015-09-01

    Full Text Available Bimetallic catalysts containing a series of Co/W at 40/10, 30/20, 20/30 and 10/40 wt% supported on MgO with a total metal content of 50 wt% were prepared and used for the catalytic decomposition of methane to COx-free hydrogen and multi-walled carbon nanotubes (MWCNTs. The solid fresh and exhausted catalysts were characterized structurally and chemically through XRD, TPR, BET, TGA, TEM and Raman spectroscopy. The 40%Co–10%W/MgO catalyst exhibited the highest activity for the production of both hydrogen and MWCNTs. The formation of a large amount of non-interacted Co3O4 species is considered as the main reason for the catalyst superiority in its activity. On the contrary, catalysts formulations of 20%Co–30%W and 10%Co–40%W demonstrated the formation of a large amount of hardly reducible CoWO4 and MgWO4 particles causing lower activity of these catalysts toward methane decomposition as evidenced through the XRD and TPR results.

  10. Organic Carbonates: Efficient Extraction Solvents for the Synthesis of HMF in Aqueous Media with Cerium Phosphates as Catalysts.

    Science.gov (United States)

    Dibenedetto, Angela; Aresta, Michele; di Bitonto, Luigi; Pastore, Carlo

    2016-01-01

    We describe a process for the selective conversion of C6 -polyols into 5-hydroxymethylfurfural (5-HMF) in biphasic systems of organic carbonate/water (OC/W), with cerium(IV) phosphates as catalysts. Different reaction parameters such as the OC/W ratio, catalyst loading, reaction time, and temperature, were investigated for the dehydration of fructose. Under the best reaction conditions, a yield of 67.7 % with a selectivity of 93.2 % was achieved at 423 K after 6 h of reaction using [(Ce(PO4)1.5 (H2 O)(H3 O)0.5 (H2 O)0.5)] as the catalyst. A maximum yield of 70 % with the same selectivity was achieved after 12 h. At the end of the reaction, the catalyst was removed by centrifugation, the organic phase was separated from water and evaporated in vacuo (with solvent recovery), and solid 5-HMF was isolated (purity >99 %). The recovery and reuse of the catalyst and the relationship between the structure of the OC and the efficiency of the extraction are discussed. The OC/W system influences the lifetime of the catalysts positively compared to only water.

  11. Organic Carbonates: Efficient Extraction Solvents for the Synthesis of HMF in Aqueous Media with Cerium Phosphates as Catalysts.

    Science.gov (United States)

    Dibenedetto, Angela; Aresta, Michele; di Bitonto, Luigi; Pastore, Carlo

    2016-01-01

    We describe a process for the selective conversion of C6 -polyols into 5-hydroxymethylfurfural (5-HMF) in biphasic systems of organic carbonate/water (OC/W), with cerium(IV) phosphates as catalysts. Different reaction parameters such as the OC/W ratio, catalyst loading, reaction time, and temperature, were investigated for the dehydration of fructose. Under the best reaction conditions, a yield of 67.7 % with a selectivity of 93.2 % was achieved at 423 K after 6 h of reaction using [(Ce(PO4)1.5 (H2 O)(H3 O)0.5 (H2 O)0.5)] as the catalyst. A maximum yield of 70 % with the same selectivity was achieved after 12 h. At the end of the reaction, the catalyst was removed by centrifugation, the organic phase was separated from water and evaporated in vacuo (with solvent recovery), and solid 5-HMF was isolated (purity >99 %). The recovery and reuse of the catalyst and the relationship between the structure of the OC and the efficiency of the extraction are discussed. The OC/W system influences the lifetime of the catalysts positively compared to only water. PMID:26676974

  12. Microwave absorbing properties and magnetic properties of different carbon nanotubes

    Institute of Scientific and Technical Information of China (English)

    2009-01-01

    The microwave absorbing properties and magnetic properties of as-grown Fe-filled carbon nanotubes (CNTs), annealed Fe-filled CNTs, and multi-walled CNTs were studied. Vibrating sample magnetometer results showed that the annealed Fe-filled CNTs have the weakest coercivity and strongest saturation magnetization among the three types CNTs, due to the presence of more ferromagnetic α-Fe nanowires. After annealing, the values increased to 291.0 Oe and 28.0 emu/g and the samples showed excellent microwave absorbing properties. The reflection loss was over 5 dB between 11.6 GHz and 18 GHz with a maximum value of 10.8 dB for annealed Fe-filled CNTs (1.1 wt%)/epoxy composite.

  13. Microwave absorbing properties and magnetic properties of different carbon nanotubes

    Institute of Scientific and Technical Information of China (English)

    GUI XuChun; WANG KunLin; WEI JinQuan; L(U) RuiTao; SHU QinKe; JIA Yi; WANG Chen; ZHU HongWei; WU DeHai

    2009-01-01

    The microwave absorbing properties and magnetic properties of as-grown Fe-filled carbon nanotubes (CNTs), annealed Fe-filled CNTs, and multi-walled CNTs were studied. Vibrating sample magnetometer results showed that the annealed Fe-filled CNTs have the weakest coercivity and strongest saturation magnetization among the three types CNTs, due to the presence of more ferromagnetic α-Fe nanowires.After annealing, the values increased to 291.00e and 28.0 emu/g and the samples showed excellent microwave absorbing properties. The reflection loss was over 5 dB between 11.6 GHz and 18 GHz with a maximum value of 10.8 dB for annealed Fe-filled CNTs (1.1 wt%)/epoxy composite.

  14. Effect of Different Catalyst Deposition Technique on Aligned Multiwalled Carbon Nanotubes Grown by Thermal Chemical Vapor Deposition

    Directory of Open Access Journals (Sweden)

    Mohamed Shuaib Mohamed Saheed

    2014-01-01

    Full Text Available The paper reported the investigation of the substrate preparation technique involving deposition of iron catalyst by electron beam evaporation and ferrocene vaporization in order to produce vertically aligned multiwalled carbon nanotubes array needed for fabrication of tailored devices. Prior to the growth at 700°C in ethylene, silicon dioxide coated silicon substrate was prepared by depositing alumina followed by iron using two different methods as described earlier. Characterization analysis revealed that aligned multiwalled carbon nanotubes array of 107.9 µm thickness grown by thermal chemical vapor deposition technique can only be achieved for the sample with iron deposited using ferrocene vaporization. The thick layer of partially oxidized iron film can prevent the deactivation of catalyst and thus is able to sustain the growth. It also increases the rate of permeation of the hydrocarbon gas into the catalyst particles and prevents agglomeration at the growth temperature. Combination of alumina-iron layer provides an efficient growth of high density multiwalled carbon nanotubes array with the steady growth rate of 3.6 µm per minute for the first 12 minutes and dropped by half after 40 minutes. Thicker and uniform iron catalyst film obtained from ferrocene vaporization is attributed to the multidirectional deposition of particles in the gaseous form.

  15. Gold catalysts supported on nanosized iron oxide for low-temperature oxidation of carbon monoxide and formaldehyde

    Science.gov (United States)

    Tang, Zheng; Zhang, Weidong; Li, Yi; Huang, Zuming; Guo, Huishan; Wu, Feng; Li, Jinjun

    2016-02-01

    This study aimed to optimize synthesis of gold catalyst supported on nanosized iron oxide and to evaluate the activity in oxidation of carbon monoxide and formaldehyde. Nanosized iron oxide was prepared from a colloidal dispersion of hydrous iron oxide through a dispersion-precipitation method. Gold was adsorbed onto nanosized iron oxide under self-generated basic conditions. Characterization results indicate that the iron oxide consisted of hematite/maghemite composite with primary particle sizes of 6-8 nm. Gold was highly dispersed on the surface of the support. The catalysts showed good activity in the oxidation of airborne carbon monoxide and formaldehyde. The optimal pH for their synthesis was ∼7. The catalytic performance could be enhanced by extending the adsorption time of gold species on the support within 21 h. The optimized catalyst was capable of achieving complete oxidation of 1% carbon monoxide at -20 °C and 33% conversion of 450 ppm formaldehyde at ambient temperature. The catalyst may be applicable to indoor air purification.

  16. A "catalyst switch" Strategy for the sequential metal-free polymerization of epoxides and cyclic Esters/Carbonate

    KAUST Repository

    Zhao, Junpeng

    2014-06-24

    A "catalyst switch" strategy was used to synthesize well-defined polyether-polyester/polycarbonate block copolymers. Epoxides (ethylene oxide and/or 1,2-butylene oxide) were first polymerized from a monoalcohol in the presence of a strong phosphazene base promoter (t-BuP4). Then an excess of diphenyl phosphate (DPP) was introduced, followed by the addition and polymerization of a cyclic ester (ε-caprolactone or δ-valerolactone) or a cyclic carbonate (trimethylene carbonate), where DPP acted as both the neutralizer of phosphazenium alkoxide (polyether chain end) and the activator of cyclic ester/carbonate. This work has provided a one-pot sequential polymerization method for the metal-free synthesis of block copolymers from monomers which are suited for different types of organic catalysts. © 2014 American Chemical Society.

  17. Tungsten carbide/porous carbon composite as superior support for platinum catalyst toward methanol electro-oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Jiang, Liming [School of Chemical Engineering and Technology, Harbin Institute of Technology, Harbin 150001 (China); Fu, Honggang, E-mail: fuhg@vip.sina.com [School of Chemical Engineering and Technology, Harbin Institute of Technology, Harbin 150001 (China); Key Laboratory of Functional Inorganic Material Chemistry, Heilongjiang University, Harbin 150080 (China); Wang, Lei; Mu, Guang; Jiang, Baojiang; Zhou, Wei; Wang, Ruihong [Key Laboratory of Functional Inorganic Material Chemistry, Heilongjiang University, Harbin 150080 (China)

    2014-01-01

    Graphical abstract: The WC nanoparticles are well dispersed in the carbon matrix. The size of WC nanoparticles is about 30 nm. It can be concluded that tungsten carbide and carbon composite was successfully prepared by the present synthesis conditions. - Highlights: • The WC/PC composite with high specific surface area was prepared by a simple way. • The Pt/WC/PC catalyst has superior performance toward methanol electro-oxidation. • The current density for methanol electro-oxidation is as high as 595.93 A g{sup −1} Pt. • The Pt/WC/PC catalyst shows better durability and stronger CO electro-oxidation. • The performance of Pt/WC/PC is superior to the commercial Pt/C (JM) catalyst. - Abstract: Tungsten carbide/porous carbon (WC/PC) composites have been successfully synthesized through a surfactant assisted evaporation-induced-assembly method, followed by a thermal treatment process. In particular, WC/PC-35-1000 composite with tungsten content of 35% synthesized at the carbonized temperature of 1000 °C, exhibited a specific surface area (S{sub BET}) of 457.92 m{sup 2} g{sup −1}. After loading Pt nanoparticles (NPs), the obtained Pt/WC/PC-35-1000 catalyst exhibits the highest unit mass electroactivity (595.93 A g{sup −1} Pt) toward methanol electro-oxidation, which is about 2.6 times as that of the commercial Pt/C (JM) catalyst. Furthermore, the Pt/WC/PC-35-1000 catalyst displays much stronger resistance to CO poisoning and better durability toward methanol electrooxidation compared with the commercial Pt/C (JM) catalyst. The high electrocatalytic activity, strong poison-resistivity and good stability of Pt/WC/PC-35-1000 catalyst are attributed to the porous structures and high specific surface area of WC/PC support could facilitate the rapid mass transportation. Moreover, synergistic effect between WC and Pt NPs is favorable to the higher catalytic performance.

  18. Feasibility study of various sulphonation methods for transforming carbon nanotubes into catalysts for the esterification of palm fatty acid distillate

    International Nuclear Information System (INIS)

    Highlights: • First report on the production of biodiesel from low-value industrial by-product using sulphonated MWCNTs as catalyst. • Various sulphonation methods were used to transform MWCNTs into catalysts. • SO3H were successfully grafted on the surface of MWCNTs, which resulted in a high biodiesel yield and reuse capacity. • The maximum FAME yield by sulphonated MWCNTs was higher than for other popular solid acid catalysts. - Abstract: Sulphonated multi-walled carbon nanotubes were synthesised and utilised as catalysts to transform palm fatty acid distillate, the low-value by-product of palm oil refineries, into the more valuable product of biodiesel. The most common method to prepare carbon-based solid acid catalysts is thermal treatment with concentrated sulphuric acid, which is a time-consuming and energy-intensive process. Therefore, the feasibility of other sulphonation methods, such as the in situ polymerisation of acetic anhydride and sulphuric acid, the thermal decomposition of ammonium sulphate and the in situ polymerisation of poly(sodium4-styrenesulphonate), were examined in this study. The esterification reaction was performed at 170 °C for 3 h at a methanol to palm fatty acid distillate ratio of 20 and catalyst loading of 2 wt% in a pressurised reactor. The fatty acid methyl esters yields achieved by the sulphonated multi-walled carbon nanotubes prepared via thermal treatment with concentrated sulphuric acid, the in situ polymerisation of acetic anhydride and sulphuric acid, the thermal decomposition of ammonium sulphate and the in situ polymerisation of poly(sodium4-styrenesulphonate) were 78.1%, 85.8%, 88.0% and 93.4%, respectively. All catalysts could maintain a high catalytic activity even during the fifth cycle. Among the sulphonation methods, the in situ polymerisation of poly(sodium4-styrenesulphonate) produced the catalyst with the highest acid group density. In addition, the resonance structures of the benzenesulphonic acid

  19. The electrochemical properties of carbon nanotubes and carbon XC-72R and their application as Pt supports

    Directory of Open Access Journals (Sweden)

    MAJA D. OBRADOVIĆ

    2010-10-01

    Full Text Available The electrocatalytic behavior of reduced nicotinamide adenine di-nucleotide (NADH was studied at the surface of a rutin biosensor, using various electrochemical methods. According to the results, the rutin biosensor had a strongly electrocatalytic effect on the oxidation of NADH with the overpotential being decreased by about 450 mV as compared to the process at a bare glassy carbon electrode, GCE. The results of an investigation of two samples of commercial multi-walled carbon nanotubes and a sample of carbon black, in the raw and activated state, were presented in the lecture. The activation of the carbon materials led to the formation of an abundance of oxygen-containing functional groups on the surface, an increased electrochemically active surface area, an enhanced charge storage ability and a promotion of the electron-transfer kinetics. It was presented that the morphology of the carbon nanotubes is important for the electrochemical properties, because nanotubes with a higher proportion of edge and defect sites showed faster electron transfer and pseudocapacitive redox kinetics. Modification of oxidized nanotubes by ethylenediamine and wrapping by poly(diallyldimethylammonium chloride led to a decrease in the electrochemically active surface area and to reduced electron-transfer kinetics. Pt nanoparticles prepared by the microwave-assisted polyol method were deposited at the investigated carbon materials. A much higher efficiency of Pt deposition was observed on the modified CNTs than on the activated CNTs. The activity of the synthesized catalyst toward electrochemical oxygen reduction was almost the same as the activity of the commercial Pt/XC-72 catalyst.

  20. Preparation of carbon nanoparticles and nanofibers by a simple microwave based method and studying the field emission properties

    International Nuclear Information System (INIS)

    Research highlights: → A novel and simple microwave based method for preparation of carbon nanostructures were developed. → The mw-plasma method can produce catalyst nanoparticles from a solid metallic source. → The resulting nanostructure exhibit good field emission (FE) properties. → Deposition of nanoparticles through the mw-plasma method improves field emission properties. - Abstract: A novel, simple and fast method for preparation of graphitic nanostructures such as nanofibers and nanospheres which uses a standard microwave oven is described. In this method polystyrene is used as carbon source and a solid metal such as nickel or iron provides both the trigger to initiate the plasma, as well as a source for sputtering catalyst particles which are required for formation of nanofibers. The mechanism of this process is discussed through analysis of different properties of the resulting products, by examining the effect of changing the microwave processing time and the nature of the metallic trigger/catalyst source. The effect of morphology of nanoparticles (nanofibers vs. nanospheres), as well as the effect of trigger/catalyst material and the deposition method on electron field emission properties of these samples, are also investigated.

  1. Reforming performance of a plasma-catalyst hybrid converter using low carbon fuels

    International Nuclear Information System (INIS)

    The reforming performance of a plasma-catalyst hybrid converter using different low carbon fuels was investigated. The methodology was to use arc from spark discharge combined with an appropriate oxygen/carbon molar ratio (O2/C) and feeding rate of the supplied mixture. To enhance the mixing and reforming reaction, a gas intake swirl was generated by inducing the mixture tangentially into the reaction chamber. The required energy for fuel processing was provided by heat released through the oxidation of the air-fuel mixture. The reforming temperature as well as the effect of steam addition on the hydrogen production was studied. The results showed that reformate gas temperature had a profound effect on the overall reaction. The H2/(CO + CO2) ratio reformed by both methane and propane was shown to increase with temperature and that the optimum ratio was obtained when reforming methane under 650 deg. C. The conversion efficiency of the fuel was also shown to increase with increasing temperature. The best thermal efficiency of 72.01% was obtained near 750 deg. C. The theoretical equilibrium calculations and the experimental results were compared.

  2. Studies on metal catalysts and carbon materials for fuel cell applications

    Science.gov (United States)

    Zhang, Gaixia

    As a potential candidate for an environmentally benign and highly efficient electric power generation technology, proton exchange membrane fuel cells (PEMFC) are now attracting great interest for various applications. The main objective of this project has been to investigate the interfacial interaction of Pt nanoparticles with their carbon supports, so as to determine ways to optimise the catalyst electrode and to increase its catalytic activity, thereby enhancing PEM fuel cell performance. We first studied the interfacial interaction (leading to adhesion) of Pt nanoparticles evaporated onto untreated and Ar+-treated highly oriented pyrolytic graphite surfaces, with, respectively, low and high surface defect densities; HOPG was used as a model for carbon nanotubes (CNTs) and carbon fibers. We found that those Pt nanoparticles have very weak interactions with their pristine carbon material supports, with no evidence of compound formation between them. Our analysis, however, indicated that the adhesion of Pt nanoparticles to their supports can be enhanced, using ion beams, plasmas, or other treatments to establish defects on the carbon substrate surface. In addition, by using multicomponent XPS analysis with symmetric lineshapes for each Pt4f spectral component (4f7/2,5/2), we attributed the component peaks to the existence of (i) surface oxidation on the platinum nanoparticles, and different electronic configurations of (ii) surface and (iii) bulk Pt atoms. One way of enhancing strong adhesion between them is by chemical functionalization of the support. Using mixed H2SO4/HNO3 acid treatments, we have characterized the surface chemistry of functionalized carbon fiber paper by combining infrared, Raman and X-ray photoelectron spectroscopies, to give new insights into the often-used oxidation of graphene-containing materials. We have, for the first time, demonstrated the presence of transient O-, N- and S-containing species during the oxidation process, as well as

  3. Production of biodiesel fuel from canola oil with dimethyl carbonate using an active sodium methoxide catalyst prepared by crystallization.

    Science.gov (United States)

    Kai, Takami; Mak, Goon Lum; Wada, Shohei; Nakazato, Tsutomu; Takanashi, Hirokazu; Uemura, Yoshimitsu

    2014-07-01

    In this study, a novel method for the production of biodiesel under mild conditions using fine particles of sodium methoxide formed in dimethyl carbonate (DMC) is proposed. Biodiesel is generally produced from vegetable oils by the transesterification of triglycerides with methanol. However, this reaction produces glycerol as a byproduct, and raw materials are not effectively utilized. Transesterification with DMC has recently been studied because glycerol is not formed in the process. Although solid-state sodium methoxide has been reported to be inactive for this reaction, the catalytic activity dramatically increased with the preparation of fine catalyst powders by crystallization. The transesterification of canola oil with DMC was studied using this catalyst for the preparation of biodiesel. A conversion greater than 96% was obtained at 65°C for 2h with a 3:1M ratio of DMC and oil and 2.0 wt% catalyst.

  4. Synthesis of single-walled carbon nanotubes using induction thermal plasma technology with different catalysts: thermodynamic and experimental studies

    International Nuclear Information System (INIS)

    The effects of the type and quantity of three catalyst mixtures (i.e. Ni-Y2O3, Ni-Co-Y2O3, and Ni-Mo-Y2O3) on single-walled carbon nanotubes (SWCNT) synthesis by induction thermal plasma process have been examined in order to evaluate their individual influences on SWCNT production. Thermodynamic calculations, in gas and particularly in liquid solution phases, have also been performed to better understand the effects of the catalysts on the production of SWCNT. Characterization of the synthesized SWCNT by different techniques including Raman spectroscopy, high resolution scanning electron microscopy (HRSEM) imaging and thermogravimetric analysis (TGA) clearly indicated that the best quality of SWCNT was achieved using Ni-Co-Y2O3 catalyst mixture in the feedstock.

  5. Ultrasonically treated multi-walled carbon nanotubes (MWCNTs) as PtRu catalyst supports for methanol electrooxidation

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Chunwei; Hu, Xinguo; Wang, Dianlong; Dai, Changsong [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China); Zhang, Liang; Jin, Haibo [School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081 (China); Agathopoulos, Simeon [Department of Materials Science and Engineering, University of Ioannina, GR-451 10 Ioannina (Greece)

    2006-09-29

    In the quest of fabricating supported catalysts, experimental results of transmission electron microscopy, Raman and infrared spectroscopy indicate that ultrasonic treatment effectively functionalizes multi-walled carbon nanotubes (MWCNTs), endowing them with groups that can act as nucleation sites which can favor well-dispersed depositions of PtRu clusters on their surface. Ultrasonic treatment seems to be superior than functionalization via regular refluxing. This is confirmed by the determination of the electrochemistry active surface area (ECA) and the CO-tolerance performance of the PtRu catalysts, measured by adsorbed CO-stripping voltammetry in 0.5M sulfuric acid solution, and the real surface area of the PtRu catalysts, evaluated by Brunauer-Emmett-Teller (BET) measurements. Finally, the effectiveness for methanol oxidation is assessed by cyclic voltammetry (CV) in a sulfuric acid and methanol electrolyte. (author)

  6. Production of biodiesel fuel from canola oil with dimethyl carbonate using an active sodium methoxide catalyst prepared by crystallization.

    Science.gov (United States)

    Kai, Takami; Mak, Goon Lum; Wada, Shohei; Nakazato, Tsutomu; Takanashi, Hirokazu; Uemura, Yoshimitsu

    2014-07-01

    In this study, a novel method for the production of biodiesel under mild conditions using fine particles of sodium methoxide formed in dimethyl carbonate (DMC) is proposed. Biodiesel is generally produced from vegetable oils by the transesterification of triglycerides with methanol. However, this reaction produces glycerol as a byproduct, and raw materials are not effectively utilized. Transesterification with DMC has recently been studied because glycerol is not formed in the process. Although solid-state sodium methoxide has been reported to be inactive for this reaction, the catalytic activity dramatically increased with the preparation of fine catalyst powders by crystallization. The transesterification of canola oil with DMC was studied using this catalyst for the preparation of biodiesel. A conversion greater than 96% was obtained at 65°C for 2h with a 3:1M ratio of DMC and oil and 2.0 wt% catalyst. PMID:24813567

  7. N,P-Codoped Carbon Networks as Efficient Metal-free Bifunctional Catalysts for Oxygen Reduction and Hydrogen Evolution Reactions.

    Science.gov (United States)

    Zhang, Jintao; Qu, Liangti; Shi, Gaoquan; Liu, Jiangyong; Chen, Jianfeng; Dai, Liming

    2016-02-01

    The high cost and scarcity of noble metal catalysts, such as Pt, have hindered the hydrogen production from electrochemical water splitting, the oxygen reduction in fuel cells and batteries. Herein, we developed a simple template-free approach to three-dimensional porous carbon networks codoped with nitrogen and phosphorus by pyrolysis of a supermolecular aggregate of self-assembled melamine, phytic acid, and graphene oxide (MPSA/GO). The pyrolyzed MPSA/GO acted as the first metal-free bifunctional catalyst with high activities for both oxygen reduction and hydrogen evolution. Zn-air batteries with the pyrolyzed MPSA/GO air electrode showed a high peak power density (310 W g(-1) ) and an excellent durability. Thus, the pyrolyzed MPSA/GO is a promising bifunctional catalyst for renewable energy technologies, particularly regenerative fuel cells. PMID:26709954

  8. Effect of Modification of SBA-15 by Carbon Films on Textural and Catalytic Properties of Supported Cobalt Catalysts%SBA-15的孔壁碳膜修饰对钴基催化剂结构与催化性能的影响

    Institute of Scientific and Technical Information of China (English)

    朱海燕; 周朝华; 马兰; 程振兴; 沈俭一

    2011-01-01

    Carbon coated mesoporous SBA-15, named SBA-15C, was obtained from as-synthesized SBA-15 after graphitization in inert gas. With SBA-15 and SBA-15C as supports and cobalt nitrate aqueous solution as precursor, the supported cobalt-based catalyst samples were prepared by a wet impregnation method. The catalyst samples were characterized by X-ray diffraction, N2 physisorption, temperature-programmed reduction, and NH3 microcalorimetric adsorption. The results suggested that upon doping the inner walls of SBA-15 with carbon, the hexagonal ordered mesoporous framework was retained while the surface area decreased a little and the thickness of pore wall increased. The supported cobalt-based catalyst retained the mesoporous characteristics with decreased surface area and pore volume. The average particle size of CO3O4 on SBA-15C was smaller than that on SBA-15, which suggested that the existence of carbon improved the dispersion of CO3O4 particles. However, the modification of SBA-15 with carbon films did not seem to increase the reducibility of CO3O4. Both Co/SBA-15 and Co/SBA-15C exhibited high selectivity for Cs+ hydrocarbons (-80%), but Co/SBA-15C showed higher stability in the F-T synthesis reactions.%在惰性气体中焙烧SBA-15制得孔壁被碳修饰的SBA- 15C样品,以它和SBA-15为载体,采用等量浸渍法制备了负载型Co基催化剂,并运用X射线衍射、N2物理吸附、程序升温还原、NH3吸附量热等手段对样品进行了表征.结果表明,SBA- 15C仍保持原有的六方有序的中孔结构,但其孔壁经碳修饰后发生增厚,比表面积略有下降.Co的负载使得SBA-15和SBA-15C样品的孔径基本不变,但比表面积和孔体积下降,仍保持其中孔分子筛的特征.CO3O4在SBA- 15C上的晶粒较小,但还原度较低,表明碳的存在有利于Co物种的分散.比较了Co/SBA- 15和Co/SBA-15C上的费托合成反应性能,发现两者对C5+的选择性均较高(达80%左右),但Co/SBA- 15C

  9. Analyzing the influence of high electrode potentials on intrinsic properties of catalyst coated membranes using impedance spectroscopy

    Science.gov (United States)

    Alink, Robert; Schüßler, Martina; Pospischil, Maximilian; Erath, Denis; Gerteisen, Dietmar

    2016-09-01

    Catalyst layers (CLs) with varying ionomer contents are produced using a stencil coating and screen printing technique. The optimum ionomer content of 31-34 wt% confirms the findings of other groups and performance is found to be independent of production technique. A new CL impedance transition line model is developed and fitted to in-situ data. The results indicate that the protonic contact resistance between CL and membrane is an important factor for the used transfer-decal process, especially for CLs with low ionomer loading. When subjected to potentials higher than 1.2 V, an increased performance is observed for low ionomer loading CLs. It is found that by applying the high potential to the electrode a significantly increased proton conductivity is counteracting and superimposing the loss of electrochemical surface area (ECSA) due to carbon corrosion. After aging, the performance of the 15 wt% CL is at the same level as the 31-34 wt% ionomer content CLs at the beginning of life, even though the ECSA is reduced due to carbon corrosion or platinum dissolution. The findings indicate that for the optimization of the ionomer loading, either the changing wetting properties or the redistribution of ionomer during lifetime have to be taken into account.

  10. REFORMULATION OF COAL-DERIVED TRANSPORTATION FUELS: SELECTIVE OXIDATION OF CARBON MONOXIDE ON METAL FOAM CATALYSTS

    Energy Technology Data Exchange (ETDEWEB)

    Mr. Paul Chin; Dr. Xiaolei Sun; Professor George W. Roberts; Professor James J. Spivey; Mr. Amornmart Sirijarhuphan; Dr. James G. Goodwin, Jr.; Dr. Richard W. Rice

    2002-12-31

    Several different catalytic reactions must be carried out in order to convert hydrocarbons (or alcohols) into hydrogen for use as a fuel for polyelectrolyte membrane (PEM) fuel cells. Each reaction in the fuel-processing sequence has a different set of characteristics, which influences the type of catalyst support that should be used for that particular reaction. A wide range of supports are being evaluated for the various reactions in the fuel-processing scheme, including porous and non-porous particles, ceramic and metal straight-channel monoliths, and ceramic and metal monolithic foams. These different types of support have distinctly different transport characteristics. The best choice of support for a given reaction will depend on the design constraints for the system, e.g., allowable pressure drop, and on the characteristics of the reaction for which the catalyst is being designed. Three of the most important reaction characteristics are the intrinsic reaction rate, the exothermicity/endothermicity of the reaction, and the nature of the reaction network, e.g., whether more than one reaction takes place and, in the case of multiple reactions, the configuration of the network. Isotopic transient kinetic analysis was used to study the surface intermediates. The preferential oxidation of low concentrations of carbon monoxide in the presence of high concentrations of hydrogen (PROX) is an important final step in most fuel processor designs. Data on the behavior of straight-channel monoliths and foam monolith supports will be presented to illustrate some of the factors involved in choosing a support for this reaction.

  11. Physico-Chemical and Catalytic Properties of Mesoporous CuO-ZrO2 Catalysts

    Directory of Open Access Journals (Sweden)

    Sulaiman N. Basahel

    2016-04-01

    Full Text Available Mesoporous CuO-ZrO2 catalysts were prepared and calcined at 500 °C. The performance of the synthesized catalysts for benzylation of benzene using benzyl chloride was studied. The bare support (macroporous ZrO2 offered 45% benzyl chloride conversion after reaction time of 10 h at 75 °C. Significant increase in benzyl chloride conversion (98% was observed after CuO loading (10 wt. % on porous ZrO2 support. The conversion was decreased to 80% with increase of CuO loading to 20 wt. %. Different characterization techniques (XRD, Raman, diffuse reflectance UV-vis, N2-physisorption, H2-TPR, XPS and acidity measurements were used to evaluate physico-chemical properties of CuO-ZrO2 catalysts; the results showed that the surface and structural characteristics of the ZrO2 phase as well as the interaction between CuO-ZrO2 species depend strongly on the CuO content. The results also indicated that ZrO2 support was comprised of monoclinic and tetragonal phases with macropores. An increase of the volume of monoclinic ZrO2 phase was observed after impregnation of 10 wt. % of CuO; however, stabilization of tetragonal ZrO2 phase was noticed after loading of 20 wt. % CuO. The presence of low-angle XRD peaks indicates that mesoscopic order is preserved in the calcined CuO-ZrO2 catalysts. XRD reflections due to CuO phase were not observed in case of 10 wt. % CuO supported ZrO2 sample; in contrast, the presence of crystalline CuO phase was observed in 20 wt. % CuO supported ZrO2 sample. The mesoporous 10 wt. % CuO supported ZrO2 catalyst showed stable catalytic activity for several reaction cycles. The observed high catalytic activity of this catalyst could be attributed to the presence of a higher number of dispersed interactive CuO (Cu2+-O-Zr4+ species, easy reducibility, and greater degree of accessible surface Lewis acid sites.

  12. Effects of catalyst support and chemical vapor deposition condition on synthesis of multi-walled carbon nanocoils

    Science.gov (United States)

    Suda, Yoshiyuki; Iida, Tetsuo; Takikawa, Hirofumi; Harigai, Toru; Ue, Hitoshi; Umeda, Yoshito

    2016-02-01

    Multi-walled carbon nanocoil (MWCNC) is a carbon nanotube (CNT) with helical shape. We have synthesized MWCNCs and MWCNTs hybrid by chemical vapor deposition (CVD). MWCNCs are considered to be a potential material in nanodevices, such as electromagnetic wave absorbers and field emitters. It is very important to take into account the purity of MWCNCs. In this study, we aimed to improve the composition ratio of MWCNCs to MWCNTs by changing catalyst preparation and CVD conditions. As a catalyst, Fe2O3/zeolite was prepared by dissolving Fe2O3 fine powder and Y-type zeolite (catalyst support material) in ethanol with an Fe density of 0.5wt.% and with a zeolite density of 3.5wt.%. The catalyst-coated Si substrate was transferred immediately onto a hotplate and was heated at 80°C for 5 min. Similarly, Fe2O3/Al2O3, Co/zeolite/Al2O3, Co/zeolite, and Co/Al2O3 were prepared. The effect of the difference of the composite catalysts on synthesis of MWCNCs was considered. The CVD reactor was heated in a tubular furnace to 660-790°C in a nitrogen atmosphere at a flow rate of 1000 ml/min. Subsequently, acetylene was mixed with nitrogen at a flow rate ratio of C2H2/N2 = 0.02-0.1. The reaction was kept under these conditions for 10 min. MWCNTs and MWCNCs were well grown by the catalysts of Co/zeolite and Co/Al2O3. The composition ratio of MWCNCs to MWCNTs was increased by using a combination of zeolite and Al2O3. The highest composition ratio of MWCNCs to MWCNTs was 12%.

  13. Methanation of carbon dioxide on Ni/ZrO2-Al2O3 catalysts: Effects of ZrO2 promoter and preparation method of novel ZrO2-Al2O3 carrier

    Institute of Scientific and Technical Information of China (English)

    Mengdie Cai; Jie Wen; Wei Chu; Xueqing Cheng; Zejun Li

    2011-01-01

    The novel nickel-based catalysts with a nickel content of 12 wt% were prepared with the zirconia-alumina composite as the supports. The new carriers, ZrO2 improved alumina, were synthesized by three methods, i.e., impregnation-precipitation, co-precipitation, and impregnation method. The catalytic properties of these catalysts were investigated in the methanation of carbon dioxide, and the samples were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscope (XPS), temperature-programmed reduction (TPR) and temperature-programmed desorption (TPD) techniques. The new catalysts showed higher catalytic activity and better stability than Ni/γ-AI2O3. Furthermore, as a support for new nickel catalyst, the ZrO2-AI2O3 composite prepared by the impregnation-precipitation method was more efficient than the other supports in the methanation of carbon dioxide. The highly dispersed zirconium oxide on the surface of γ-Al2O3 inhibited the formation of nickel aluminate-like phase, which was responsible for the better dispersion of Ni species and easier reduction of NiO species, leading to the enhanced catalytic performance of corresponding catalyst.

  14. Pyrazole Supported Zinc(II Benzoates as Catalysts for the Ring Opening Copolymerization of Cyclohexene Oxide and Carbon Dioxide

    Directory of Open Access Journals (Sweden)

    Mapudumo L. Lephoto

    2016-01-01

    Full Text Available The bis(pyrazolezinc(II benzoate complexes bis(3,5-diphenylpyrazolezinc(II benzoate (1, bis(3,5-diphenylpyrazolezinc(II 3,5-dinitrobenzoate (2, bis(3,5-diphenylpyrazolezinc(II 4-hydroxybenzoate (3, and bis(3,5-di-tert-butylpyrazolezinc(II 2-chlorobenzoate (4 were synthesized from the reaction of 3,5-diphenylpyrazole (L1 or 3,5-di-tert-butylpyrazole (L2, zinc(II acetate and the appropriate benzene carboxylic acid. The molecular structure of complex 2 confirmed that these zinc(II benzoate complexes adopt a 4-coordinate tetrahedral geometry. All four complexes were screened as catalysts for the copolymerization of carbon dioxide (CO2 and cyclohexene oxide (CHO and were found to be active for the formation of poly(cyclohexene carbonate (PCHC at CO2 pressures as low as 1.0 MPa under solvent-free conditions and without the use of a co-catalyst. At some reaction condition, most of the catalysts produced PCHC with high carbonate content of up to 98% and a good amount of cyclic cyclohexene carbonate (CCHC. The copolymers produced have low to moderate molecular weights (5200–12300 g/mol and with polydispersity indices that vary from 1.19 to 2.50. Matrix Assisted Laser Desorption/Ionization-Time of Flight Mass Spectra (MALDI-TOF MS of these copolymers showed they have benzoate and hydroxyl end groups.

  15. Activity of platinum/carbon and palladium/carbon catalysts promoted by Ni2 P in direct ethanol fuel cells.

    Science.gov (United States)

    Li, Guoqiang; Feng, Ligang; Chang, Jinfa; Wickman, Björn; Grönbeck, Henrik; Liu, Changpeng; Xing, Wei

    2014-12-01

    Ethanol is an alternative fuel for direct alcohol fuel cells, in which the electrode materials are commonly based on Pt or Pd. Owing to the excellent promotion effect of Ni2 P that was found in methanol oxidation, we extended the catalyst system of Pt or Pd modified by Ni2 P in direct ethanol fuel cells. The Ni2 P-promoted catalysts were compared to commercial catalysts as well as to reference catalysts promoted with only Ni or only P. Among the studied catalysts, Pt/C and Pd/C modified by Ni2 P (30 wt %) showed both the highest activity and stability. Upon integration into the anode of a homemade direct ethanol fuel cell, the Pt-Ni2 P/C-30 % catalyst showed a maximum power density of 21 mW cm(-2) , which is approximately two times higher than that of a commercial Pt/C catalyst. The Pd-Ni2 P/C-30 % catalyst exhibited a maximum power density of 90 mW cm(-2) . This is approximately 1.5 times higher than that of a commercial Pd/C catalyst. The discharge stability on both two catalysts was also greatly improved over a 12 h discharge operation.

  16. 官能化碳纳米管负载Ru催化山梨醇氢解制备低碳二元醇%Effect of modified groups of carbon nanotubes on catalytic properties of Ru/CNTs catalysts for hydrogenolysis of sorbitol

    Institute of Scientific and Technical Information of China (English)

    董慧焕; 郭星翠; 秦张峰; 韩生; 牟新东

    2015-01-01

    以不同官能化碳纳米管(原始MCN、氨基化AMCN和石墨化GMCN等)作为载体,通过浸渍法制备了Ru/CNTs催化剂,并应用于山梨醇氢解制1,2-丙二醇和乙二醇反应中. 利用XRD、HRTEM、XPS和ICP-AES等方法对催化剂进行了表征,考察了官能团性质、碱助剂等因素对山梨醇氢解性能的影响. 结果表明,与Ru/MCN或Ru/GMCN相比较,Ru/AMCN催化剂对山梨醇氢解有更高的活性,在205℃、5. 0 MPa氢压条件下,以Ca(OH)2 为添加剂,山梨醇的转化率可达99. 5%,1,2-丙二醇(1,2-PD)和乙二醇(EG)的总产率为47. 7%. 催化剂重复利用五次,催化活性无明显下降.%Ruthenium catalysts supported on carbon nanotubes with different functional groups ( MCN, AMCN and GMCN ) were prepared by incipient wetness impregnation with ultrasonic-assistance and used for the hydrogenolysis of sorbitol. The catalysts were characterized by X-ray diffraction ( XRD ) , HRTEM, X-ray photoelectron spectroscopy ( XPS) and ICP-AES. The effects of functional group species, and base additives on the catalytic performance of Ru/CNTs in the sorbitol hydrogenolysis reaction were investigated. Nearly 99. 5%of sorbitol conversion and 47 . 7% total yield of ethylene glycol and 1 , 2-propanediol ( 1 , 2-PD ) could be achieved over Ru/AMCN under mild reaction conditions (205℃, 5. 0 MPa), using Ca(OH)2 as additive. The conversion of sorbitol and the selectivity to ethylene glycol ( EG ) and 1 , 2-propanediol ( 1 , 2-PD ) did not decrease over the five repeated runs, which confirmed that the Ru/AMCN catalyst exhibited high stability in the aqueous hydrogenolysis of sorbitol to glycols.

  17. Mechanistic aspects of the copolymerization reaction of carbon dioxide and epoxides, using a chiral salen chromium chloride catalyst.

    Science.gov (United States)

    Darensbourg, Donald J; Yarbrough, Jason C

    2002-06-01

    The air-stable, chiral (salen)Cr(III)Cl complex (3), where H(2)salen = N,N'-bis(3,5-di-tert-butyl-salicylidene)-1,2-cyclohexene diamine, has been shown to be an effective catalyst for the coupling of cyclohexene oxide and carbon dioxide to afford poly(cyclohexenylene carbonate), along with a small quantity of its trans-cyclic carbonate. The thus produced polycarbonate contained >99% carbonate linkages and had a M(n) value of 8900 g/mol with a polydispersity index of 1.2 as determined by gel permeation chromatography. The turnover number (TON) and turnover frequency (TOF) values of 683 g of polym/g of Cr and 28.5 g of polym/g of Cr/h, respectively for reactions carried out at 80 degrees C and 58.5 bar pressure increased by over 3-fold upon addition of 5 equiv of the Lewis base cocatalyst, N-methyl imidazole. Although this chiral catalyst is well documented for the asymmetric ring-opening (ARO) of epoxides, in this instance the copolymer produced was completely atactic as illustrated by (13)C NMR spectroscopy. Whereas the mechanism for the (salen)Cr(III)-catalyzed ARO of epoxides displays a squared dependence on [catalyst], which presumably is true for the initiation step of the copolymerization reaction, the rate of carbonate chain growth leading to copolymer or cyclic carbonate formation is linearly dependent on [catalyst]. This was demonstrated herein by way of in situ measurements at 80 degrees C and 58.5 bar pressure. Hence, an alternative mechanism for copolymer production is operative, which is suggested to involve a concerted attack of epoxide at the axial site of the chromium(III) complex where the growing polymer chain for epoxide ring-opening resides. Preliminary investigations of this (salen)Cr(III)-catalyzed system for the coupling of propylene oxide and carbon dioxide reveal that although cyclic carbonate is the main product provided at elevated temperatures, at ambient temperature polycarbonate formation is dominant. A common reaction pathway for

  18. X-ray fluorescence as a method of monitoring metal catalyst content during the purification of carbon nanotubes

    Science.gov (United States)

    Cavness, Brandon; Heimbecker, Joshua; Velasquez, Joe; Williams, S.

    2012-02-01

    There have been several studies that suggest that catalyst metals in carbon nanotubes (CNTs) may pose a health threat. As there are many potential applications of CNTs in medicine, it is important to be able to quantitatively determine the amount of metal catalyst contained in a CNT sample. The relative catalyst content of carbon nanotube samples synthesized via arc-discharge has been determined at various stages of the purification process using X-ray fluorescence (XRF) analysis. Purification was achieved by immersing samples in heated nitric acid. The intensities of the nickel K α X-rays were studied to determine the relative catalyst content in the samples. Scanning electron microscopy (SEM) images of purified nanotubes have been compared to the images of a sample that has been irradiated by 0-15 keV bremsstrahlung in order to determine if the XRF analysis of the nanotubes is in any way destructive. No obvious structural defects were observed as the result of irradiation.

  19. Carbon corrosion of proton exchange membrane fuel cell catalyst layers studied by scanning transmission X-ray microscopy

    Science.gov (United States)

    Hitchcock, Adam P.; Berejnov, Viatcheslav; Lee, Vincent; West, Marcia; Colbow, Vesna; Dutta, Monica; Wessel, Silvia

    2014-11-01

    Scanning Transmission X-ray Microscopy (STXM) at the C 1s, F 1s and S 2p edges has been used to investigate degradation of proton exchange membrane fuel cell (PEM-FC) membrane electrode assemblies (MEA) subjected to accelerated testing protocols. Quantitative chemical maps of the catalyst, carbon support and ionomer in the cathode layer are reported for beginning-of-test (BOT), and end-of-test (EOT) samples for two types of carbon support, low surface area carbon (LSAC) and medium surface area carbon (MSAC), that were exposed to accelerated stress testing with upper potentials (UPL) of 1.0, 1.2, and 1.3 V. The results are compared in order to characterize catalyst layer degradation in terms of the amounts and spatial distributions of these species. Pt agglomeration, Pt migration and corrosion of the carbon support are all visualized, and contribute to differing degrees in these samples. It is found that there is formation of a distinct Pt-in-membrane (PTIM) band for all EOT samples. The cathode thickness shrinks due to loss of the carbon support for all MSAC samples that were exposed to the different upper potentials, but only for the most aggressive testing protocol for the LSAC support. The amount of ionomer per unit volume significantly increases indicating it is being concentrated in the cathode as the carbon corrosion takes place. S 2p spectra and mapping of the cathode catalyst layer indicates there are still sulfonate groups present, even in the most damaged material.

  20. Effect of catalyst concentration on size, morphology and optical properties of silica nanoparticles

    Science.gov (United States)

    Arora, Ekta; Ritu, Kumar, Sacheen; Kumar, Dinesh

    2016-05-01

    Today, nanomaterials play a key role in various fields such as electronics, aerospace, pharmaceuticals and biomedical because of their unique physical, chemical and biological properties which are different from bulk materials. Nano sized silica particles have gained the prominent position in scientific research and have wide applications. The sol-gel method is the best method to synthesize silica nanoparticles because of its potential to produce monodispersed with narrow size distribution at mild conditions. The silica nanoparticles were obtained by hydrolysis of tetraethyl orthosilicate (TEOS) in ethanol act as solvent. The synthesized nanoparticles were characterized by Field Emission Scanning electron Microscope (FE-SEM), UV Spectrometer. The smallest size of silica particles is around 150nm examined by using FE-SEM. The optical properties and band structure was analyzed using UV-visible spectroscopy which is found to be increase by reducing the size of particles. Concentration effect of catalyst on the size, morphology and optical properties were analyzed.

  1. Structure, Properties, Functionalization, and Applications of Carbon Nanohorns.

    Science.gov (United States)

    Karousis, Nikolaos; Suarez-Martinez, Irene; Ewels, Christopher P; Tagmatarchis, Nikos

    2016-04-27

    Carbon nanohorns (sometimes also known as nanocones) are conical carbon nanostructures constructed from an sp(2) carbon sheet. Nanohorns require no metal catalyst in their synthesis, and can be produced in industrial quantities. They provide a realistic and useful alternative to carbon nanotubes, and possibly graphene, in a wide range of applications. They also have their own unique behavior due to their specific conical morphology. However, their research and development has been slowed by several factors, notably during synthesis, they aggregate into spherical clusters ∼100 nm in diameter, blocking functionalization and treatment of individual nanocones. This limitation has recently been overcome with a new approach to separating these "dahlia-like" clusters into individual nanocones. In this review, we describe the structure, synthesis, and topology of carbon nanohorns, and provide a detailed review of nanohorn chemistry. PMID:27074223

  2. Impact of carbonation on water transport properties of cementitious materials

    International Nuclear Information System (INIS)

    Carbonation is a very well-known cementitious materials pathology. It is the major cause of reinforced concrete structures degradation. It leads to rebar corrosion and consequent concrete cover cracking. In the framework of radioactive waste management, cement-based materials used as building materials for structures or containers would be simultaneously submitted to drying and atmospheric carbonation. Although scientific literature regarding carbonating is vast, it is clearly lacking information about the influence of carbonation on water transport properties. This work then aimed at studying and understanding the change in water transport properties induced by carbonation. Simultaneously, the representativeness of accelerated carbonation (in the laboratory) was also studied. (author)

  3. De-oxygenation of CO2 by using Hydrogen, Carbon and Methane over Alumina-Supported Catalysts

    Directory of Open Access Journals (Sweden)

    R.Y. Raskar

    2012-06-01

    Full Text Available The de-oxygenation of CO2 was explored by using hydrogen, methane, carbon etc., over alumina supported catalysts. The alumina-supported ruthenium, rhodium, platinum, molybdenum, vanadium and magnesium catalysts were first reduced in hydrogen atmosphere and then used for the de-oxygenation of CO2. Furthermore, experimental variables for the de-oxygenation of CO2 were temperature (range 50 to 650 oC, H2/CO2 mole ratios (1.0 to 5, and catalyst loading (0.5 to 10 wt %. During the de-oxygenation of CO2 with H2 or CH4 or carbon, conversion of CO2, selectivity to CO and CH4 were estimated. Moreover, 25.4 % conversion of CO2 by hydrogen was observed over 1 wt% Pt/Al2O3 catalyst at 650 oC with 33.8 % selectivity to CH4. However, 8.1 to 13.9 % conversion of CO2 was observed over 1 wt% Pt/Al2O3 catalyst at 550 oC in the presence of both H2 and CH4. Moreover, 42.8 to 79.4 % CH4 was converted with 9 to 23.1 % selectivity to CO. It was observed that the de-oxygenation of CO2 by hydrogen, carbon and methane produced carbon, CO and CH4. © 2012 BCREC UNDIP. All rights reservedReceived: 6th February 2012; Revised: 23rd April 2012; Accepted: 24th April 2012[How to Cite: R. Y. Raskar, K. B. Kale, A. G. Gaikwad. (2011. De-oxygenation of CO2 by using Hydrogen, Carbon and Methane over Alumina-Supported Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 7 (1: 59-69.  doi:10.9767/bcrec.7.1.1631.59-69][How to Link / DOI: http://dx.doi.org/10.9767/bcrec.7.1.1631.59-69 ] | View in 

  4. A parametric study of methane decomposition into carbon nanotubes over 8Co-2Mo/Al2O3 catalyst

    Institute of Scientific and Technical Information of China (English)

    Siang-Piao Chai; Choon-Ming Seah; Abdul Rahman Mohamed

    2011-01-01

    The effects of reaction temperature,partial pressure of methane,catalyst weight and gas hourly space velocity(GHSV)on methane decomposition were reported.The decomposition reaction was performed in a vertical fixed-bed reactor over 8Co-2Mo/Al2O3 catalyst.The experimental results show that these four process parameters studied had vital effects on carbon yield.As revealed by the electron microscopy and Raman spectroscopy analyses,the reaction temperature and GHSV governed the average diameter,the diameter distribution and the degree of graphitization of the synthesized carbon nanotubes(CNTs).Also,an evidence is presented to show that higher temperatures and higher GHSV favored the formation of better-graphitized CNTs with larger diameters.

  5. Microwave axial dielectric properties of carbon fiber

    Science.gov (United States)

    Hong, Wen; Xiao, Peng; Luo, Heng; Li, Zhuan

    2015-10-01

    Randomly distributed carbon fibers (CFs) reinforced epoxy resin composites are prepared by the pouring method, the dielectric properties of CF composites with different fiber content and length have been performed in the frequency range from 8.2 to 12.4 GHz. The complex permittivity of the composite increases with the fiber length, which is attributed to the decrease of depolarization field, and increases with the volume fraction, which is attributed to the increase of polarization. A formula, based on the theory of Reynolds-Hugh, is proposed to calculate the effective permittivity of CF composites, and validated by the experiments. The proposed formula is further applied to derive the axial permittivity of CF and analyze the effect of fiber length on the axial permittivity.

  6. One Dimensional Graphitic Carbon Nitrides as Effective Metal-Free Oxygen Reduction Catalysts

    OpenAIRE

    Muhammad Tahir; Nasir Mahmood; Jinghan Zhu; Asif Mahmood; Butt, Faheem K.; Syed Rizwan; Imran Aslam; Tanveer, M.; Faryal Idrees; Imran Shakir; Chuanbao Cao; Yanglong Hou

    2015-01-01

    To explore the effect of morphology on catalytic properties of graphitic carbon nitride (GCN), we have studied oxygen reduction reaction (ORR) performance of two different morphologies of GCN in alkaline media. Among both, tubular GCN react with dissolved oxygen in the ORR with an onset potential close to commercial Pt/C. Furthermore, the higher stability and excellent methanol tolerance of tubular GCN compared to Pt/C emphasizes its suitability for fuel cells.

  7. 3-Orders-of-magnitude density control of single-walled carbon nanotube networks by maximizing catalyst activation and dosing carbon supply.

    Science.gov (United States)

    Han, Zhao Jun; Levchenko, Igor; Yick, Samuel; Ostrikov, Kostya Ken

    2011-11-01

    Tailoring the density of random single-walled carbon nanotube (SWCNT) networks is of paramount importance for various applications, yet it remains a major challenge due to the insufficient catalyst activation in most growth processes. Here we report on a simple and effective method to maximise the number of active catalyst nanoparticles using catalytic chemical vapor deposition (CCVD). By modulating short pulses of acetylene into a methane-based CCVD growth process, the density of SWCNTs is dramatically increased by up to three orders of magnitude without increasing the catalyst density and degrading the nanotube quality. In the framework of a vapor-liquid-solid model, we attribute the enhanced growth to the high dissociation rate of acetylene at high temperatures at the nucleation stage, which can be effective in both supersaturating the larger catalyst nanoparticles and overcoming the nanotube nucleation energy barrier of the smaller catalyst nanoparticles. These results are highly relevant to numerous applications of random SWCNT networks in next-generation energy, sensing and biomedical devices.

  8. Improvement of carbon fiber surface properties using electron beam irradiation

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    Carbon fiber-reinforced advance composites have been used for struetural applications, mainly on account of their mechanical properties. The main factor for a good mechanical performance of carbon fiber-reinforced composite is the interfacial interaction between its components, which are carbon fiber and polymeric matrix. The aim of this study is to improve the surface properties of the carbon fiber using ionizing radiation from an electron beam to obtain better adhesion properties in the resultant composite. EB radiation was applied on the carbon fiber itself before preparing test specimens for the mechanical tests. Experimental results showed that EB irradiation improved the tensile strength of carbon fiber samples. The maximum value in tensile strength was reached using doses of about 250kGy. After breakage, the morphology aspect of the tensile specimens prepared with irradiated and non-irradiated carbon fibers were evaluated. SEM micrographs showed modifications on the carbon fiber surface.

  9. Ruthenium Nanoparticles Loaded on Carbon as Effective Catalyst for Highly Selective Hydrogenation of 4,4'-Methylenedianiline

    Institute of Scientific and Technical Information of China (English)

    DU Wen-qiang; RONG Ze-ming; LU Xin-yi; WANG Yi-fan; LU Lian-hai; QU Jing-ping

    2012-01-01

    Supported Ru-based catalysts,prepared by a surfactant-stabilized colloidal method,exhibited a good selectivity to bis(4-aminocyclohexyl)methane via the hydrogenation of 4,4'-methylenedianiline.Transmission electron microscopy(TEM) and X-ray diffraction(XRD) characterization showed Ru nanoparticles were well-dispersed on activated carbon,leading to the high activity and selectivity to the product.

  10. Characterization of surface carbon formed during the conversion of methane to benzene over Mo/H-ZSM-5 catalysts

    NARCIS (Netherlands)

    Weckhuysen, B.M.; Rosynek, Michael P.; Lunsford, Jack H.

    2001-01-01

    During the conversion of methane to benzene in the absence of oxygen over a 2 wt% Mo/H-ZSM-5 catalyst at 700 °C, three different types of surface carbon have been observed by X-ray photoelectron spectroscopy: adventitious or graphitic-like C (284.6 eV), carbidic-like C (282.7 eV), and hydrogen-poor

  11. Reducing-Agent-Free Instant Synthesis of Carbon-Supported Pd Catalysts in a Green Leidenfrost Droplet Reactor and Catalytic Activity in Formic Acid Dehydrogenation

    OpenAIRE

    Dong-Wook Lee; Min-Ho Jin; Young-Joo Lee; Ju-Hyoung Park; Chun-Boo Lee; Jong-Soo Park

    2016-01-01

    The development of green synthesis methods for supported noble metal catalysts remains important challenges to improve their sustainability. Here we first synthesized carbon-supported Pd catalysts in a green Leidenfrost droplet reactor without reducing agents, high-temperature calcination and reduction procedures. When the aqueous solution containing Pd nitrate precursor, carbon support, and water is dripped on a hot plate, vapor layer is formed between a solution droplet and hot surface, whi...

  12. Phosphate-Doped Carbon Black as Pt Catalyst Support: Co-catalytic Functionality for Dimethyl Ether and Methanol Electro-oxidation

    DEFF Research Database (Denmark)

    Yin, Min; Huang, Yunjie; Li, Qingfeng;

    2014-01-01

    Niobium-phosphate-doped (NbP-doped) carbon blacks were prepared as the composite catalyst support for Pt nanoparticles. Functionalities of the composite include intrinsic proton conductivity, surface acidity, and interfacial synergistic interactions with methanol and dimethyl ether (DME). The sup......Niobium-phosphate-doped (NbP-doped) carbon blacks were prepared as the composite catalyst support for Pt nanoparticles. Functionalities of the composite include intrinsic proton conductivity, surface acidity, and interfacial synergistic interactions with methanol and dimethyl ether (DME...

  13. Quality improvement of single-walled carbon nanotubes by doping B in Fe/MgO catalyst

    International Nuclear Information System (INIS)

    We demonstrate that the quality of the as-grown single-walled carbon nanotubes (SWCNTs) can be effectively improved by the addition of the B ingredient in the Fe/MgO catalyst. The as-grown SWCNTs were characterized by scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM) and Raman spectroscopy. The SWCNTs prepared by the pure Fe/MgO catalyst have relatively low graphite crystallinity and are coated by much amorphous carbon. The intensity ratio of the D- and G-bands (ID/IG) in Raman spectra is relatively high (0.098 for laser 532 nm and 0.075 for laser 785 nm). The SWCNTs grown from the Fe/MgO catalyst doped with 0.1 part of B have more regular graphite structure with little amorphous carbon. The ID/IG values reduced remarkably (0.041 for laser 532 nm and 0.040 for laser 785 nm). The effect would be attributed to the inhibitory action of the doped B on the formation of radical hydrocarbon species for the formation of SWCNTs.

  14. Design of Pt/Carbon Xerogel Catalysts for PEM Fuel Cells

    Directory of Open Access Journals (Sweden)

    Nathalie Job

    2015-01-01

    Full Text Available The design of efficient catalytic layers of proton exchange membrane fuel cells (PEMFCs requires the preparation of highly-loaded and highly-dispersed Pt/C catalysts. During the last few years, our work focused on the preparation of Pt/carbon xerogel electrocatalysts, starting from simple impregnation techniques that were further optimized via the strong electrostatic adsorption (SEA method to reach high dispersion and a high metal weight fraction. The SEA method, which consists of the optimization of the precursor/support electrostatic impregnation through an adequate choice of the impregnation pH with regard to the support surface chemistry, leads to very well-dispersed Pt/C samples with a maximum 8 wt.% Pt after drying and reduction under H2. To increase the metal loading, the impregnation-drying-reduction cycle of the SEA method can be repeated several times, either with fresh Pt precursor solution or with the solution recycled from the previous cycle. In each case, a high dispersion (Pt particle size ~3 nm is obtained. Finally, the procedure can be simplified by combination of the SEA technique with dry impregnation, leading to no Pt loss during the procedure.

  15. Carbon nitride nanosheet-supported porphyrin: a new biomimetic catalyst for highly efficient bioanalysis.

    Science.gov (United States)

    Deng, Shengyuan; Yuan, Peixin; Ji, Xubo; Shan, Dan; Zhang, Xueji

    2015-01-14

    A highly efficient biomimetic catalyst was fabricated based on ultrathin carbon nitride nanosheets (C3N4)-supported cobalt(II) proto-porphyrin IX (CoPPIX). The periodical pyridinic nitrogen units in C3N4 backbone could serve as electron donors for great affinity with Co(2+) in PPIX, which resembled the local electronic structure as vitamin B12 and heme cofactor of hemoglobin. UV-vis kinetics and electrochemistry revealed its competitive (electro)catalysis with conventional peroxidase, while X-ray photoelectron spectroscopy and theoretical calculations suggest that the rehybridization of Co 3d with N orbitals from the backside can result in significant changes in enthalpy and charge density, which greatly promoted the activity of CoPPIX. The prepared nanocatalyst was further conjugated with streptavidin via multiple amines on the edge plane of C3N4 for facile tagging. Using biotinylated molecular beacon as the capture probe, a sensitive electrochemiluminescence-based DNA assay was developed via the electroreduction of H2O2 as the coreactant after the hairpin unfolded by the target, exhibiting linearity from 1.0 fM to 0.1 nM and a detection limit of 0.37 fM. Our results demonstrate a new paradigm to rationally design inexpensive and durable biomimics for electrochemiluminescence quenching strategy, showing great promise in bioanalytical applications.

  16. Selective Dehydration of Sorbitol to Isosorbide over Sulfonated Activated Carbon Catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Kang, Hyo Yoon; Hwang, Dong Won; Hwang, Young Kyu; Hwang, Jin-Soo; Chang, Jong-San [Korea Research Institute of Chemical Technology (KRICT), Daejeon (Korea, Republic of)

    2013-04-15

    A sulfonated activated carbon (AC-SO{sub 3}H) was used as a solid acid catalyst for dehydration of sorbitol to isosorbide and its catalytic performance was compared with the commercial solid acid such as acidic ion exchange resin, Amberlyst-36, and sulfated copper oxide. The catalytic performance with 100% sorbitol conversion and 52% isosorbide selectivity was obtained over AC-SO{sub 3}H at 423.15 K. Although AC-SO{sub 3}H possessed only 0.5 mmol/g of sulfur content, it showed the similar dehydration activity of sorbitol to isosorbide with Amberlyst-36 (5.4 mmol/g) at 423.15 K. Based on the high thermal and chemical stability of AC-SO{sub 3}H, one-step reactive distillation, where isosorbide separation can be carried out simultaneously with sorbitol dehydration, was tried to increase the recovery yield of isosorbide from sorbitol. The reactive distillation process using AC-SO{sub 3}H, the turnover number of AC-SO{sub 3}H was 4 times higher than the conventional two-step process using sulfuric acid.

  17. Inkjet printing of carbon supported platinum 3-D catalyst layers for use in fuel cells

    Science.gov (United States)

    Taylor, André D.; Kim, Edward Y.; Humes, Virgil P.; Kizuka, Jeremy; Thompson, Levi T.

    We present a method of using inkjet printing (IJP) to deposit catalyst materials onto gas diffusion layers (GDLs) that are made into membrane electrode assemblies (MEAs) for polymer electrolyte fuel cell (PEMFC). Existing ink deposition methods such as spray painting or screen printing are not well suited for ultra low (Monarch 700, Black Pearls 2000, etc.). Our ink jet printed MEAs with catalyst loadings of 0.020 mg Pt cm -2 have shown Pt utilizations in excess of 16,000 mW mg -1 Pt which is higher than our traditional screen printed MEAs (800 mW mg -1 Pt). As a further demonstration of IJP versatility, we present results of a graded distribution of Pt/C catalyst structure using standard Johnson Matthey (JM) catalyst. Compared to a continuous catalyst layer of JM Pt/C (20% Pt), the graded catalyst structure showed enhanced performance.

  18. Chemically Synthesised Pt Particles on Surface Oxidized Carbon Nanotubes as an Effective Catalyst for Direct Methanol Fuel Cell

    Institute of Scientific and Technical Information of China (English)

    Mohammad; yari; Sajjad; Sadaghat; Sharehjini

    2007-01-01

    1 Results The synthesis, physical characterization and electrochemical analysis of Pt particles prepared using the surface oxidized carbon nanotubes prepared by chemically anchoring Pt onto the surface of the CNTs with 2.0 mol/L HNO3 by refluxing for 10 h to introduce surface functional groups.The particles of Pt are synthesized by reduction with sodium borohydride of H2PtCl6. The electro-oxidation of liquid methanol of this catalyst as a thin layer on glassy carbon electrode is investigated at room te...

  19. CCVD synthesis of carbon nanotubes from (Mg,Co,Mo)O catalysts: influence of the proportions of cobalt and molybdenum

    OpenAIRE

    Flahaut, Emmanuel; Peigney, Alain; Bacsa, Wolfgang; Bacsa, Revathi; Laurent, Christophe

    2004-01-01

    International audience Carbon nanotubes have been synthesised by catalytic chemical vapour deposition of a H2-CH4 mixture (18 mol% CH4) over (Mg,Co,Mo)O catalysts. The total amount of cobalt and molybdenum has been kept constant at 1 cat% and the proportion of molybdenum with respect to cobalt has been varied from x(Mo) = 0.25-1.0. This variation has important effects on both the yield and the nature (number of walls, straight walls or bamboo-like structures) of the carbon nanotubes. It al...

  20. Synthesis of the Multinuclear Cobaloxime Complexes via Click Chemistry as Catalysts for the Formation of Cyclic Carbonates from Carbon Dioxide and Epoxides

    Indian Academy of Sciences (India)

    Ahmet Kilic; Armagan Keles; Emine Aytar; Mustafa Durgun; Mahmut Ulusoy

    2015-09-01

    In this study, the structurally similar multinuclear cobaloxime complexes based on dioxime ligands were synthesized and characterized as trinuclear complexes with respect to varied axial groups. The multinuclear cobaloxime complexes were characterized by 1H, 13C-NMR, FT-IR, UV-Vis, LC-MS spectra, melting point and magnetic susceptibility measurements. These multinuclear cobaloxime complexes have been successfully applied to the synthesis of cyclic carbonates from CO2 and epoxides under optimized conditions and with-out using any solvent. All multinuclear cobaloxime complexes obtained by click chemistry are good catalysts for the cycloaddition of CO2 to different epoxides in the presence of pyridine as a co-catalyst. Additionally, the effects of epoxides, bases, temperature, pressure, and time on the yield of cyclic carbonates were investigated.

  1. Assessment of the ethanol oxidation activity and durability of Pt catalysts with or without a carbon support using Electrochemical Impedance Spectroscopy

    Science.gov (United States)

    Saleh, Farhana S.; Easton, E. Bradley

    2014-01-01

    We compared the stability and performance of 3 commercially available Johnson Matthey catalysts with various Pt loadings (20, 40 and 100%) using two different accelerated durability testing (ADT) protocols. The various Pt-loaded catalysts were tested by means of a series of intermittent life tests (1, 200, 400, 1000, 2000, 3000 and 4000 cycles). The electrochemical surface area (ECSA) loss of electrode was investigated by electrochemical technique (CV). The use of EIS as an accelerated-testing protocol distinctly elucidates the extent of degradation of Johnson Matthey catalysts with various Pt loading. Using EIS, it was possible to show that Pt-black catalyst layers suffer from increased electronic resistance over the course of ADT which is not observed when a corrosion stable carbon support is present. The effect of Pt loading was further elucidated by comparing the electrocatalytic activity of the catalyst layers towards ethanol oxidation reaction (EOR). The catalyst layer with the lowest Pt loading showed the enhanced EOR performance.

  2. CATALYTIC WET PEROXIDE OXIDATION OF HYDROQUINONE WITH Co(Ⅱ)/ACTIVE CARBON CATALYST LOADED IN STATIC BED

    Institute of Scientific and Technical Information of China (English)

    LI Chunxiang; YAN Yongsheng; XU Wanzhen

    2008-01-01

    Catalysts based on Co(Ⅱ) supported on active carbon were prepared and loaded in static bed.The hydroquinone wouid be degraded completely after treated by Catalytic wet peroxide oxidation method with Co(Ⅱ)/active carbon catalyst.After activate treatment, the active carbon was immerged in cobaltoas nitrate solution, then put into a drying oven, Co(Ⅱ) could be loaded on the micro-surface of carbon.Taking the static bed as the equipment, the absorption of active carbon and catalysis of Co(Ⅱ) was used to reduce activation energy of hydroquinone.Thus hydroquinone could be drastically degraded and the effluent can be drained under the standard.Referring to Fenton reaction mechanism, experiment had been done to study the heterogeneous catalyzed oxidation mechanism of Co(Ⅱ).The degradation rate of hydroquinone effluent could be achieved to 92% when treated in four columns at H2O2 concentration 10%, reaction temperature 40℃, pH 5 and reaction time 2.5h.

  3. CATALYTIC WET PEROXIDE OXIDATION OF HYDROQUINONE WITH Co(II)/ACTIVE CARBON CATALYST LOADED IN STATIC BED

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    Catalysts based on Co(II) supported on active carbon were prepared and loaded in static bed. The hydroquinone would be degraded completely after treated by Catalytic wet peroxide oxidation method with Co(II)/active carbon catalyst. After activate treatment, the active carbon was immerged in cobaltous nitrate solution, then put into a drying oven, Co(II) could be loaded on the micro-surface of carbon. Taking the static bed as the equipment, the absorption of active carbon and catalysis of Co(II) was used to reduce activation energy of hydroquinone. Thus hydroquinone could be drastically degraded and the effluent can be drained under the standard. Referring to Fenton reaction mechanism, experiment had been done to study the heterogeneous catalyzed oxidation mechanism of Co(II). The degradation rate of hydroquinone effluent could be achieved to 92% when treated in four columns at H2O2 concentration 10%, reaction temperature 40℃ , pH 5 and reaction time 2.5h.

  4. Alkali promoted molybdenum (IV) sulfide based catalysts, development and characterization for alcohol synthesis from carbon monoxide and hydrogen

    Science.gov (United States)

    Molina, Belinda Delilah

    For more than a century transition metal sulfides (TMS) have been the anchor of hydro-processing fuels and upgrading bitumen and coal in refineries worldwide. As oil supplies dwindle and environmental laws become more stringent, there is a greater need for cleaner alternative fuels and/or synthetic fuels. The depletion of oil reserves and a rapidly increasing energy demand worldwide, together with the interest to reduce dependence on foreign oil makes alcohol production for fuels and chemicals via the Fischer Tropsch synthesis (FTS) very attractive. The original Fischer-Tropsch (FT) reaction is the heart of all gas-to-liquid technologies; it creates higher alcohols and hydrocarbons from CO/H2 using a metal catalyst. This research focuses on the development of alkali promoted MoS2-based catalysts to investigate an optimal synthesis for their assistance in the production of long chain alcohols (via FTS) for their use as synthetic transportation liquid fuels. Properties of catalytic material are strongly affected by every step of the preparation together with the quality of the raw materials. The choice of a laboratory method for preparing a given catalyst depends on the physical and chemical characteristics desired in the final composition. Characterization methods of K0.3/Cs0.3-MoS2 and K0.3 /Cs0.3-Co0.5MoS2 catalysts have been carried out through Scanning Electron Microscopy (SEM), BET porosity and surface analysis, Transmission Electron Microscopy (TEM) and X-Ray Diffraction (XRD). Various characterization methods have been deployed to correlate FTS products versus crystal and morphological properties of these heterogeneous catalysts. A lab scale gas to liquid system has been developed to evaluate its efficiency in testing FT catalysts for their production of alcohols.

  5. Central composite design approach towards optimization of flamboyant pods derived steam activated carbon for its use as heterogeneous catalyst in transesterification of Hevea brasiliensis oil

    International Nuclear Information System (INIS)

    Highlights: • Activated carbon was prepared from novel precursor flamboyant pods (Delonix regia). • Activation process was optimized using central composite design approach. • Prepared activated carbon at optimized condition was used as support for KOH. • Carbon based heterogeneous catalyst was used in transesterification of HBO. • Effect of catalyst loading and alcohol ratio on biodiesel yield was studied. - Abstract: The present investigation emphasises the preparation of carbon based KOH impregnated heterogeneous catalyst from flamboyant pods (Delonix regia) for the production of biodiesel from novel feedstock Hevea brasiliensis oil (HBO). Initially, carbonized char was physically activated by superheated steam and the process was optimized to study the effects of activation time and temperature by central composite design approach (CCD) using response surface methodology (RSM). Activated carbon was impregnated with KOH at four different ratios. Biodiesel production process was carried out at constant temperature 60 °C, reaction time 1 h, and 5 g of carbon based catalyst at varying quantities of catalyst loading (0.5, 2, 3.5, 5 wt%) and methanol to oil ratio (5:1–20:1). The influence of parameters on the biodiesel yield at varied condition was studied. Maximum yield of 89.3% was obtained at methanol to oil ratio 15:1 and catalyst loading 3.5 wt% and corresponding yield at same process parameters was observed to be 88.7% implying the significant activity of catalyst in reutilization. Produced biodiesel was characterized following ASTM standards. The experimental analysis confirmed that the carbonaceous catalyst developed from flamboyant pods under optimized condition is capable of transesterifying HBO into biodiesel

  6. Transport Properties of Carbon-Nanotube/Cement Composites

    NARCIS (Netherlands)

    Han, B.; Yang, Z.; Shi, X.; Yu, X.

    2012-01-01

    This paper preliminarily investigates the general transport properties (i.e., water sorptivity, water permeability, and gas permeability) of carbon-nanotube/cement composites. Carboxyl multi-walled carbon nanotubes (MWNTs) are dispersed into cement mortar to fabricate the carbon nanotubes (CNTs) rei

  7. Metal-free Ketjenblack incorporated nitrogen-doped carbon sheets derived from gelatin as oxygen reduction catalysts.

    Science.gov (United States)

    Nam, Gyutae; Park, Joohyuk; Kim, Sun Tai; Shin, Dong-bin; Park, Noejung; Kim, Youngsik; Lee, Jang-Soo; Cho, Jaephil

    2014-01-01

    Electrocatalysts facilitating oxygen reduction reaction (ORR) are vital components in advanced fuel cells and metal-air batteries. Here we report Ketjenblack incorporated nitrogen-doped carbon sheets derived from gelatin and apply these easily scalable materials as metal-free electrocatalysts for ORR. These carbon nanosheets demonstrate highly comparable catalytic activity for ORR as well as better durability than commercial Vulcan carbon supported Pt catalysts in alkaline media. Physico-chemical characterization and theoretical calculations suggest that proper combination of graphitic and pyridinic nitrogen species with more exposed edge sites effectively facilitates a formation of superoxide, [O2(ad)](-), via one-electron transfer, thus increasing catalytic activities for ORR. Our results demonstrate a novel strategy to expose more nitrogen doped edge sites by irregular stacked small sheets in developing better electrocatalysts for Zn-air batteries. These desirable architectures are embodied by an amphiphlilic gelatin mediated compatible synthetic strategy between hydrophobic carbon and aqueous water. PMID:24635744

  8. Coal-based carbons with molecular sieve properties

    Energy Technology Data Exchange (ETDEWEB)

    El-Wakil, A.M.; Youssef, A.M.; Tollan, K.A. (Mansoura Univ. (Egypt))

    1991-01-01

    Carbon molecular sieves are used extensively in gas chromatography for the separation of permanent gases and light hydrocarbons. Carbon molecular sieves also find commercial application for the manufacture of pure hydrogen from hydrogen-rich gases such as coke-oven gas, and for the separation of air by the pressure-swing adsorption technique. The objective of this investigation was to prepare carbons from Maghara coal, recently available on the commercial market. Coal-based carbons, if they possess molecular sieve properties, are superior to molecular sieve carbons from agricultural by-products because they have more satisfactory mechanical properties.

  9. Chirality specific and spatially uniform synthesis of single-walled carbon nanotubes from a sputtered Co-W bimetallic catalyst

    Science.gov (United States)

    An, Hua; Kumamoto, Akihito; Takezaki, Hiroki; Ohyama, Shinnosuke; Qian, Yang; Inoue, Taiki; Ikuhara, Yuichi; Chiashi, Shohei; Xiang, Rong; Maruyama, Shigeo

    2016-07-01

    Synthesis of single-walled carbon nanotubes (SWNTs) with well-defined atomic arrangements has been widely recognized in the past few decades as the biggest challenge in the SWNT community, and has become a bottleneck for the application of SWNTs in nano-electronics. Here, we report a selective synthesis of (12, 6) SWNTs with an enrichment of 50%-70% by chemical vapor deposition (CVD) using sputtered Co-W as a catalyst. This is achieved under much milder reduction and growth conditions than those in the previous report using transition-metal molecule clusters as catalyst precursors (Nature, 2014, 510, 522). Meanwhile, in-plane transmission electron microscopy unambiguously identified an intermediate structure of Co6W6C, which is strongly associated with selective growth. However, most of the W atoms disappear after a 5 min CVD growth, which implies that anchoring W may be important in this puzzling Co-W system.Synthesis of single-walled carbon nanotubes (SWNTs) with well-defined atomic arrangements has been widely recognized in the past few decades as the biggest challenge in the SWNT community, and has become a bottleneck for the application of SWNTs in nano-electronics. Here, we report a selective synthesis of (12, 6) SWNTs with an enrichment of 50%-70% by chemical vapor deposition (CVD) using sputtered Co-W as a catalyst. This is achieved under much milder reduction and growth conditions than those in the previous report using transition-metal molecule clusters as catalyst precursors (Nature, 2014, 510, 522). Meanwhile, in-plane transmission electron microscopy unambiguously identified an intermediate structure of Co6W6C, which is strongly associated with selective growth. However, most of the W atoms disappear after a 5 min CVD growth, which implies that anchoring W may be important in this puzzling Co-W system. Electronic supplementary information (ESI) available: Raman spectroscopy (G-band) of SWNTs grown from Co and Co-W catalyst; Kataura plot for chirality

  10. Thermal properties of graphene and nanostructured carbon materials

    Science.gov (United States)

    Balandin, Alexander A.

    2011-08-01

    Recent years have seen a rapid growth of interest by the scientific and engineering communities in the thermal properties of materials. Heat removal has become a crucial issue for continuing progress in the electronic industry, and thermal conduction in low-dimensional structures has revealed truly intriguing features. Carbon allotropes and their derivatives occupy a unique place in terms of their ability to conduct heat. The room-temperature thermal conductivity of carbon materials span an extraordinary large range -- of over five orders of magnitude -- from the lowest in amorphous carbons to the highest in graphene and carbon nanotubes. Here, I review the thermal properties of carbon materials focusing on recent results for graphene, carbon nanotubes and nanostructured carbon materials with different degrees of disorder. Special attention is given to the unusual size dependence of heat conduction in two-dimensional crystals and, specifically, in graphene. I also describe the prospects of applications of graphene and carbon materials for thermal management of electronics.

  11. Synthesis of superparamagnetic carbon nanotubes immobilized Pt and Pd pincer complexes: highly active and selective catalysts towards cyclohexane oxidation with dioxygen.

    Science.gov (United States)

    Machado, Kelly; Mishra, Jaya; Suzuki, Shinzo; Mishra, Gopal S

    2014-12-14

    Single-walled carbon nanotubes (SWNTs) with Ni/Co have been prepared using an arc discharge technique and Ni/Co-carbon composite rods in an inert atmosphere and were surface modified using 3-aminophenyl trimethoxysilane. These NH2-functionalized magnetic carbon nanotubes have been used as a novel support for Pd((II)) and Pt((II)) pincer complexes immobilized as magnetic nano-catalysts. The morphology of the support and the catalysts have been characterized by IR, EPR, SEM, TGA, TEM, XRD, AAS and EDS analysis. These magnetic nano-catalysts have been tested on the industrially important cyclohexane (Cy-hx) oxidation with O2 and significantly high TONs of 1678 to 1946 were achieved under solvent free and relatively mild conditions. The SWNTs/Pd catalyst provided the best conversion, 22.7%, but the SWNTs/Pt system also provided a good conversion of 20.7%. PMID:25340475

  12. COx-Free Hydrogen and Carbon Nanofibers Produced from Direct Decomposition of Methane on Nickel-Based Catalysts

    Institute of Scientific and Technical Information of China (English)

    Siang-Piao Chai; Sharif Hussein Sharif Zein; Abdul Rahman Mohamed

    2006-01-01

    Direct decomposition of methane was carried out using a fixed-bed reactor at 700 ℃ for the production of COx-free hydrogen and carbon nanofibers. The catalytic performance of NiO-M/SiO2catalysts (where M=AgO, CoO, CuO, FeO, MnOx and MoO) in methane decomposition was investigated.The experimental results indicate that among the tested catalysts, NiO/SiO2 promoted with CuO give the highest hydrogen yield. In addition, the examination of the most suitable catalyst support, including Al2O3, CeO2, La2O3, SiO2, and TiO2, shows that the decomposition of methane over NiO-CuO favors SiO2 support. Furthermore, the optimum ratio of NiO to CuO on SiO2 support for methane decomposition was determined. The experimental results show that the optimum weight ratio of NiO to CuO fell at 8:2(w/w) since the highest yield of hydrogen was obtained over this catalyst.

  13. Synthesis of subnanometer-diameter vertically aligned single-walled carbon nanotubes with copper-anchored cobalt catalysts.

    Science.gov (United States)

    Cui, Kehang; Kumamoto, Akihito; Xiang, Rong; An, Hua; Wang, Benjamin; Inoue, Taiki; Chiashi, Shohei; Ikuhara, Yuichi; Maruyama, Shigeo

    2016-01-21

    We synthesize vertically aligned single-walled carbon nanotubes (VA-SWNTs) with subnanometer diameters on quartz (and SiO2/Si) substrates by alcohol CVD using Cu-anchored Co catalysts. The uniform VA-SWNTs with a nanotube diameter of 1 nm are synthesized at a CVD temperature of 800 °C and have a thickness of several tens of μm. The diameter of SWNTs was reduced to 0.75 nm at 650 °C with the G/D ratio maintained above 24. Scanning transmission electron microscopy energy-dispersive X-ray spectroscopy (EDS-STEM) and high angle annular dark field (HAADF-STEM) imaging of the Co/Cu bimetallic catalyst system showed that Co catalysts were captured and anchored by adjacent Cu nanoparticles, and thus were prevented from coalescing into a larger size, which contributed to the small diameter of SWNTs. The correlation between the catalyst size and the SWNT diameter was experimentally clarified. The subnanometer-diameter and high-quality SWNTs are expected to pave the way to replace silicon for next-generation optoelectronic and photovoltaic devices. PMID:26690843

  14. Pt-free carbon-based fuel cell catalyst prepared from spherical polyimide for enhanced oxygen diffusion

    Science.gov (United States)

    Nabae, Yuta; Nagata, Shinsuke; Hayakawa, Teruaki; Niwa, Hideharu; Harada, Yoshihisa; Oshima, Masaharu; Isoda, Ayano; Matsunaga, Atsushi; Tanaka, Kazuhisa; Aoki, Tsutomu

    2016-03-01

    The development of a non-precious metal (NPM) fuel cell catalyst is extremely important to achieve globalization of polymer electrolyte fuel cells due to the cost and scarcity of platinum. Here, we report on a NPM cathode catalyst prepared by the pyrolysis of spherical polyimide nanoparticles that contain small amounts of Fe additive. 60 nm diameter Fe-containing polyimide nanoparticles were successfully synthesized by the precipitation polymerization of pyromellitic acid dianhydride and 1,3,5-tris(4-aminophenyl)benzene with Fe(acac)3 (acac = acetylacetonate) as an additive. The particles were subsequently carbonized by multistep pyrolysis to obtain the NPM catalyst while retaining the small particle size. The catalyst has good performance and promising durability for fuel cell applications. The fuel cell performance under a 0.2 MPa air atmosphere at 80 °C of 1.0 A cm‑2 at 0.46 V is especially remarkable and better than that previously reported.

  15. Activity, short-term stability (poisoning tolerance) and durability of carbon supported Pt-Pr catalysts for ethanol oxidation

    Science.gov (United States)

    Corradini, Patricia G.; Antolini, Ermete; Perez, Joelma

    2014-04-01

    Pt-Pr/C electrocatalysts were prepared by a modified formic acid method, and their activity for carbon monoxide and ethanol oxidation, their short term stability and durability were compared to that of commercial Pt/C and Pt-Sn/C (3:1) catalysts. By derivative voltammetry (DV) it was found that ethanol electro-oxidation takes place by two main pathways at different potentials. It was observed that, in the presence of Pr, ethanol electro-oxidation takes place mostly through the pathway at lower potential, which is the most interesting for fuel cell application. The Pt-Pr/C catalysts were less tolerant to poisoning by ethanol oxidation intermediate species than Pt/C. Durability test by a repetitive potential cycling under Ar atmosphere revealed a good structural stability of Pt-Pr/C catalysts. A repetitive potential cycling under CO atmosphere carried out on the Pt-Pr/C (1:1) catalyst, instead, indicated a structural change, likely by formation of a core-shell structure.

  16. Oxidation of Carbon Monoxide over Cu/CeO2 Catalysts Prepared by SMAI

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Supported Cu catalysts for low-temperature CO oxidation were prepared by solvated metal atom impregnation (SMAI). X-ray photoelectron spectroscopy (XPS) investigations indicated that the copper in all the samples was in a metallic state. XRD measurements showed that the mean diameters of Cu particles prepared by SMAI were small. Catalytical tests showed that the SMAI catalyst had high CO oxidation activity.

  17. Carbonate phosphonium salts as catalysts for the transesterification of dialkyl carbonates with diols. The competition between cyclic carbonates and linear dicarbonate products.

    Science.gov (United States)

    Selva, Maurizio; Caretto, Alessio; Noè, Marco; Perosa, Alvise

    2014-06-28

    At 90-120 °C, in the presence of methylcarbonate and bicarbonate methyltrioctylphosphonium salts as catalysts ([P8881][A]; [A] = MeOCO2 and HOCO2), the transesterification of non-toxic dimethyl- and diethyl-carbonate (DMC and DEC, respectively) with 1,X-diols (2 ≤ X ≤ 6) proceeds towards the formation of cyclic and linear products. In particular, 1,2-propanediol and ethylene glycol afford propylene- and ethylene-carbonate with selectivity and yields up to 95 and 90%, respectively; while, the reaction of DMC with higher diols such 1,3-butanediol, 2-methyl-1,3-propanediol, 1,3-propanediol, 2,2-dimethyl, 1,3-propanediol, 1,4-butanediol and 1,6-hexanediol produce linear C8-C10 dicarbonates of general formula MeOC(O)O∼∼∼OC(O)OMe as the almost exclusive products. Of note, these dicarbonate derivatives are not otherwise accessible in good yields by other conventional base catalyzed methods. Among 1,3-diols, the only exception was 2-methyl 2,4-pentandiol that yields the corresponding cyclic carbonate, i.e. 4,4,6-trimethyl-1,3-dioxan-2-one. In no one case, polycarbonates are observed. Such remarkable differences of product distributions are ascribed to the structure (branching and relative position of OH groups) of diols and to the role of cooperative (nucleophilic and electrophilic) catalysis which has been proved for onium salts. The investigated carbonate salts are not only effective in amounts as low as 0.5 mol%, but they are highly stable and recyclable. PMID:24825024

  18. CuO/CeO2 Catalysts for Selective Oxidation of Carbon Monoxide in Excess Hydrogen

    Institute of Scientific and Technical Information of China (English)

    刘春涛; 史鹏飞; 张菊香

    2004-01-01

    CuO/CeO2 catalysts were prepared by a coprecipitation method and tested for CO removal from reformed fuels via selective oxidation. The influence of the calcination temperature on the chemical compositions and catalytic performance of CuO/CeO2 catalysts were studied. It was found that CuO/CeO2 catalysts exhibit excellent CO oxidation activity and selectivity,and the complete removal of CO is attained when the catalysts are calcined at appropriate temperatures. XRD, TPR and XPS results indicate that CuO/CeO2 catalysts exhibit higher catalytic performance in CO selective oxidation due to the strong interaction between copper oxide and cerium dioxide, which promotes the dispersion and hydrogen reduction activity of copper.

  19. Influence of HF acid catalyst concentration on properties of aerogel low-k thin films

    Science.gov (United States)

    Gaikwad, A. S.; Gupta, S. A.; Mahajan, A. M.

    2016-08-01

    The effect of hydrofluoric acid (HF) catalyst concentration in coating solution on chemical, physical and structural properties of silica aerogel thin films was investigated. The aerogel films were synthesized by using a sol-gel spin coating method followed by aging in ethanol and CO2 supercritical drying. The refractive index (RI) is observed to be reduced from 1.32 to 1.13 and porosity percentage increased from 30.21% to 71.64% in accordance with increasing HF concentration. Deposition of silica aerogel was confirmed from Fourier transform infrared spectroscopy measurement. The nanoporous nature of deposited films was confirmed from field effect scanning electron microscopy and observed pore diameter is in the range of 3.33 to 6.69 nm. The nanoporous nature of the film was also validated from atomic force microscopy and root mean square roughness was observed to be increased from 2.31 nm to 3.2 nm with increasing acid catalyst concentration in the coating solution. The calculated dielectric constant from CV measurement of fabricated metal-insulator-semiconductor structure for the silica aerogel formed at 0.8 ml HF concentration is observed to be 1.73. These deposited nanoporous silica aerogel low-k films with lower k value and smaller pore size have application as interlayer dielectric materials to minimize the disadvantages of porous materials.

  20. Elastin-like recombinamer catalyst-free click gels: characterization of poroelastic and intrinsic viscoelastic properties.

    Science.gov (United States)

    González de Torre, Israel; Santos, Mercedes; Quintanilla, Luis; Testera, Ana; Alonso, Matilde; Rodríguez Cabello, José Carlos

    2014-06-01

    Elastin-like recombinamer catalyst-free click gels (ELR-CFCGs) have been prepared and characterized by modifying both a structural ELR (VKVx24) and a biofunctionalized ELR-bearing RGD cell-adhesion sequence (HRGD6) to bear the reactive groups needed to form hydrogels via a click reaction. Prior to formation of the ELR-CFCGs, azide-bearing and cyclooctyne-modified ELRs were also synthesized. Subsequent covalent crosslinking was based on the reaction between these azide and cyclooctyne groups, which takes place under physiological conditions and without the need for a catalyst. The correlation among SEM micrographs, porosity, swelling ratio, and rheological measurements have been carried out. The storage and loss moduli at 1Hz are in the range 1-10kPa and 100-1000Pa, respectively. The linear dependence of |G∗| on f(½) and the peak value of tan δ were considered to be consistent with a poroelastic mechanism dominating the frequency range 0.3-70Hz. The discrete relaxation spectrum was obtained from stress relaxation measurements (t>5s). The good fit of the relaxation modulus to decrease exponential functions suggests that an intrinsic viscoelastic mechanism dominates the transients. Several recombinamer concentrations and temperatures were tested to obtain gels with fully tuneable properties that could find applications in the biomedical field. PMID:24530853

  1. Ruthenium(0) nanoparticles supported on multiwalled carbon nanotube as highly active catalyst for hydrogen generation from ammonia-borane.

    Science.gov (United States)

    Akbayrak, Serdar; Ozkar, Saim

    2012-11-01

    Ruthenium(0) nanoparticles supported on multiwalled carbon nanotubes (Ru(0)@MWCNT) were in situ formed during the hydrolysis of ammonia-borane (AB) and could be isolated from the reaction solution by filtration and characterized by ICP-OES, XRD, TEM, SEM, EDX, and XPS techniques. The results reveal that ruthenium(0) nanoparticles of size in the range 1.4-3.0 nm are well-dispersed on multiwalled carbon nanotubes. They were found to be highly active catalyst in hydrogen generation from the hydrolysis of AB with a turnover frequency value of 329 min⁻¹. The reusability experiments show that Ru(0)@MWCNTs are isolable and redispersible in aqueous solution; when redispersed they are still active catalyst in the hydrolysis of AB exhibiting a release of 3.0 equivalents of H₂ per mole of NH₃BH₃ and preserving 41% of the initial catalytic activity even after the fourth run of hydrolysis. The lifetime of Ru(0)@MWCNTs was measured as 26400 turnovers over 29 h in the hydrolysis of AB at 25.0 ± 0.1 °C before deactivation. The work reported here also includes the kinetic studies depending on the temperature to determine the activation energy of the reaction (E(a) = 33 ± 2 kJ/mol) and the effect of catalyst concentration on the rate of the catalytic hydrolysis of AB, respectively. PMID:23113804

  2. Selective recovery of molybdenum from spent HDS catalyst using oxidative soda ash leach/carbon adsorption method

    Energy Technology Data Exchange (ETDEWEB)

    Park, Kyung Ho [Minerals and Materials Processing Division, Korea Institute of Geoscience and Mineral Resources (KIGAM), Daejeon 305-350 (Korea, Republic of); Mohapatra, D. [Minerals and Materials Processing Division, Korea Institute of Geoscience and Mineral Resources (KIGAM), Daejeon 305-350 (Korea, Republic of); Reddy, B. Ramachandra [Minerals and Materials Processing Division, Korea Institute of Geoscience and Mineral Resources (KIGAM), Daejeon 305-350 (Korea, Republic of) and Inorganic Chemistry Division, Indian Institute of Chemical Technology (CSIR), Hyderabad 500 007 (India)]. E-mail: brcreddy_iict@yahoo.com

    2006-11-16

    The petroleum refining industry makes extensive use of hydroprocessing catalysts. These catalysts contain environmentally critical and economically valuable metals such as Mo, V, Ni and Co. In the present study, a simple hydrometallurgical processing of spent hydrodesulphurization (HDS) catalyst for the recovery of molybdenum using sodium carbonate and hydrogen peroxide mixture was investigated. Recovery of molybdenum was largely dependent on the concentrations of Na{sub 2}CO{sub 3} and H{sub 2}O{sub 2} in the reaction medium, which in turn controls the pH of leach liquor and the presence of Al and Ni as impurities. Under the optimum leaching conditions (40 g L{sup -1} Na{sub 2}CO{sub 3}, 6 vol.% H{sub 2}O{sub 2}, room temperature, 1 h) about 85% recovery of Mo was achieved. The leach liquor was processed by the carbon adsorption method, which selectively adsorbs Mo at pH around 0.75. Desorption of Mo was selective at 15 vol.% NH{sub 4}OH. With a single stage contact, it was found possible to achieve >99%, adsorption and desorption efficiency. Using this method, recovery of molybdenum as MoO{sub 3} product of 99.4% purity was achieved.

  3. Selective recovery of molybdenum from spent HDS catalyst using oxidative soda ash leach/carbon adsorption method.

    Science.gov (United States)

    Park, Kyung Ho; Mohapatra, D; Reddy, B Ramachandra

    2006-11-16

    The petroleum refining industry makes extensive use of hydroprocessing catalysts. These catalysts contain environmentally critical and economically valuable metals such as Mo, V, Ni and Co. In the present study, a simple hydrometallurgical processing of spent hydrodesulphurization (HDS) catalyst for the recovery of molybdenum using sodium carbonate and hydrogen peroxide mixture was investigated. Recovery of molybdenum was largely dependent on the concentrations of Na2CO3 and H2O2 in the reaction medium, which in turn controls the pH of leach liquor and the presence of Al and Ni as impurities. Under the optimum leaching conditions (40 g L(-1) Na2CO3, 6 vol.% H2O2, room temperature, 1h) about 85% recovery of Mo was achieved. The leach liquor was processed by the carbon adsorption method, which selectively adsorbs Mo at pH around 0.75. Desorption of Mo was selective at 15 vol.% NH4OH. With a single stage contact, it was found possible to achieve >99%, adsorption and desorption efficiency. Using this method, recovery of molybdenum as MoO3 product of 99.4% purity was achieved. PMID:16860466

  4. The influence of Mn species on the SO2 removal of Mn-based activated carbon catalysts

    Science.gov (United States)

    Qu, Yi-Fan; Guo, Jia-Xiu; Chu, Ying-Hao; Sun, Ming-Chao; Yin, Hua-Qiang

    2013-10-01

    Using Mn(NO3)2 as precursor, a series of Mn-based activated carbon catalysts were prepared by ultrasound-assisted excessive impregnation method and characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and temperature programmed reduction (TPR). The influences of Mn species and nitric acid pretreatment on the removal role of SO2 were investigated. MnO and Mn3O4 coexist in catalysts calcined at 650 and 800 °C and exhibit best SO2 removal ability, whereas Mn2O3 formed in the catalyst calcined at 500 °C and shows poor activity. After treatment by nitric acid, the Cdbnd O of activated carbon support increases and the crystal size of MnO decreases, resulting in the enhancement of the catalytic activity. During reaction process, manganese oxides are gradually transferred into MnO2. And this change directly results in a decrease of activity. But the SO2 removal rate has been maintained in the range of 30-40%, indicating that MnO2 still has a certain SO2 removal ability.

  5. New Homogeneous Chromophore/Catalyst Concepts for the Solar-Driven Reduction of Carbon Dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Hopkins, Michael D. [The University of Chicago, Chicago, IL (United States)

    2015-06-22

    One of the major scientific and technical challenges of this century is to develop chemical means to store solar energy in the form of fuels. This can be accomplished by developing light-absorbing and catalytic compounds that function cooperatively to rearrange the chemical bonds of feedstocks in a way that allows solar energy to be stored and released on demand. The research conducted during this project was directed toward addressing fundamental questions that underlie the conversion of CO2 to a solar fuel using homogeneous molecular systems. The research focused particularly on developing methods for extracting the reducing equivalents for these photochemical conversions from H2, which is a renewable molecule sourced to water. The research followed two main lines. One effort focused on understanding the general principles that govern how light-absorbing molecules interact with independent H2 oxidation and CO2 reduction catalysts to produce a functional cycle for driving the energy-storing reverse water-gas-shift reaction with light. The second effort centered on developing the excited-state properties and H2 activation chemistry of tungsten–alkylidyne complexes. These chromophores were found to be powerful excited-state reducing agents, which could be incorporated into light-light-harvesting assemblies, and to hold the potential to be regenerated using H2.

  6. Promoting effect of Ir on the catalytic property of Ru/ZnO catalysts for selective hydrogenation of crotonaldehyde

    International Nuclear Information System (INIS)

    A series of ZnO supported Ru–Ir bimetal catalysts were prepared and tested for vapor-phase selective hydrogenation of crotonaldehyde. The addition of Ir could effectively promote the catalytic performance, especially the catalyst stability. A Ru–0.5Ir/ZnO catalyst showed the highest activity (a conversion of 63.3%) and selectivity to crotyl alcohol (94.4%) after 30 h reaction. The enhanced stability was attributed to the modified electronic property of Ru by the formation of RuIr alloy as the X-ray photoelectron spectroscopy results showed charge transfer from Ru to Ir, as well as the weakened surface acidity in the Ru–Ir/ZnO catalyst as evidenced by NH3 temperature-programmed desorption technique. Besides, the deactivation of the catalysts was due to the strong chemisorption of CO on the metal surface via decarbonylation reaction and deposition of organic compounds on the catalyst surface, which was characterized by CO poisoning experiment, CO temperature-programmed desorption and temperature-programmed oxidation methods.

  7. Mechanical properties of carbon nanotube/polymer composites

    OpenAIRE

    B. Arash; Wang, Q.(The University of Kansas, Lawrence, USA); Varadan, V. K.

    2014-01-01

    The remarkable mechanical properties of carbon nanotubes, such as high elastic modulus and tensile strength, make them the most ideal and promising reinforcements in substantially enhancing the mechanical properties of resulting polymer/carbon nanotube composites. It is acknowledged that the mechanical properties of the composites are significantly influenced by interfacial interactions between nanotubes and polymer matrices. The current challenge of the application of nanotubes in the compos...

  8. Highly selective hydrogenation of phenol and derivatives over a Pd@carbon nitride catalyst in aqueous media.

    Science.gov (United States)

    Wang, Yong; Yao, Jia; Li, Haoran; Su, Dangsheng; Antonietti, Markus

    2011-03-01

    Cyclohexanone is an important intermediate in the manufacture of polyamides in chemical industry, but direct selective hydrogenation of phenol to cyclohexanone under mild conditions is a challenge. We report here a catalyst made of Pd nanoparticles supported on a mesoporous graphitic carbon nitride, Pd@mpg-C(3)N(4), which was shown to be highly active and promoted the selective formation of cyclohexanone under atmospheric pressure of hydrogen in aqueous media without additives. Conversion of 99% and a selectivity higher than 99% were achieved within 2 h at 65 °C. The reaction can be accelerated at higher temperature, but even at room temperature, 99% conversion and 96% selectivity could still be obtained. The generality of the Pd@mpg-C(3)N(4) catalyst for this reaction was demonstrated by selective hydrogenation of other hydroxylated aromatic compounds with similar performance. PMID:21294506

  9. Ruthenium oxide modified titanium dioxide nanotube arrays as carbon and binder free lithium-air battery cathode catalyst

    Science.gov (United States)

    Zhao, Guangyu; Niu, Yanning; Zhang, Li; Sun, Kening

    2014-12-01

    RuO2 modified TiO2 nanotube arrays, growing on Ti foams, are used as carbon and binder free cathodes for Li-O2 batteries. The micrometer pores in Ti foams and nanometer pores in TiO2 nanotubes supply facilitated transport channels for oxygen diffusing into/out of the catalysts in discharge and charge processes. The RuO2 catalyst exhibits outstanding catalytic active toward oxygen evolution reaction (OER), which leads the charge voltage maintaining around 3.7 V all through the battery cycling. The stability of TiO2/Ti support, abundant oxygen transport path and favorable catalytic activity of RuO2 toward OER enable the Li-O2 batteries exhibiting 130 cycle discharge/charge.

  10. Clean Donor Oxidation Enhances the H2 Evolution Activity of a Carbon Quantum Dot-Molecular Catalyst Photosystem.

    Science.gov (United States)

    Martindale, Benjamin C M; Joliat, Evelyne; Bachmann, Cyril; Alberto, Roger; Reisner, Erwin

    2016-08-01

    Carbon quantum dots (CQDs) are new-generation light absorbers for photocatalytic H2 evolution in aqueous solution, but the performance of CQD-molecular catalyst systems is currently limited by the decomposition of the molecular component. Clean oxidation of the electron donor by donor recycling prevents the formation of destructive radical species and non-innocent oxidation products. This approach allowed a CQD-molecular nickel bis(diphosphine) photocatalyst system to reach a benchmark lifetime of more than 5 days and a record turnover number of 1094±61 molH2  (molNi )(-1) for a defined synthetic molecular nickel catalyst in purely aqueous solution under AM1.5G solar irradiation. PMID:27355200

  11. Chirality specific and spatially uniform synthesis of single-walled carbon nanotubes from a sputtered Co-W bimetallic catalyst.

    Science.gov (United States)

    An, Hua; Kumamoto, Akihito; Takezaki, Hiroki; Ohyama, Shinnosuke; Qian, Yang; Inoue, Taiki; Ikuhara, Yuichi; Chiashi, Shohei; Xiang, Rong; Maruyama, Shigeo

    2016-08-14

    Synthesis of single-walled carbon nanotubes (SWNTs) with well-defined atomic arrangements has been widely recognized in the past few decades as the biggest challenge in the SWNT community, and has become a bottleneck for the application of SWNTs in nano-electronics. Here, we report a selective synthesis of (12, 6) SWNTs with an enrichment of 50%-70% by chemical vapor deposition (CVD) using sputtered Co-W as a catalyst. This is achieved under much milder reduction and growth conditions than those in the previous report using transition-metal molecule clusters as catalyst precursors (Nature, 2014, 510, 522). Meanwhile, in-plane transmission electron microscopy unambiguously identified an intermediate structure of Co6W6C, which is strongly associated with selective growth. However, most of the W atoms disappear after a 5 min CVD growth, which implies that anchoring W may be important in this puzzling Co-W system. PMID:27412697

  12. Effect of impregnation protocol in the metallic sites of Pt–Ag/activated carbon catalysts for water denitration

    Energy Technology Data Exchange (ETDEWEB)

    Aristizábal, A. [Departament d’Enginyeria Química, Universitat Rovira i Virgili, Campus Sescelades, Av. Països Catalans 26, 43007 Tarragona (Spain); Contreras, S., E-mail: sandra.contreras@urv.cat [Departament d’Enginyeria Química, Universitat Rovira i Virgili, Campus Sescelades, Av. Països Catalans 26, 43007 Tarragona (Spain); Divins, N.J.; Llorca, J. [Institut de Tècniques Energètiques i Centre de Recerca en Nanoenginyeria, Universitat Politècnica de Catalunya, Diagonal 647, 08028 Barcelona (Spain); Medina, F. [Departament d’Enginyeria Química, Universitat Rovira i Virgili, Campus Sescelades, Av. Països Catalans 26, 43007 Tarragona (Spain)

    2014-04-01

    Highlights: • Mean particle size is tuned by the Pt precursor. H{sub 2}PtCl{sub 6} leads to smaller size. • H{sub 2}PtCl{sub 6} leads to higher extent of Pt–Ag particles with a composition richer in silver. • Pt(NH{sub 3}){sub 4}(NO{sub 3}){sub 2} leads to Ag{sup 0} particles and some Pt–Ag ensembles in less extent. • Nitrate and nitrite rates are linearly related to mean metal particle size. • Physical mixture of catalysts enhances N{sub 2} selectivities. - Abstract: The influence of the Pt precursor and the impregnation protocol in the catalytic behavior of 3%Pt–1.5%Ag supported on activated carbon for water denitration in a continuous reactor was studied. Pt(NH{sub 3}){sub 4}(NO{sub 3}){sub 2} and H{sub 2}PtCl{sub 6} were selected as Pt precursors. Five protocols were investigated: sequential impregnations (both sequences), co-impregnation, physical mixture of monometallic catalysts, and physical mixture of a bimetallic catalyst with a Pt monometallic catalyst. The samples were characterized by XRD, XPS, TPR, HRTEM and physisorption. It was found that the catalytic activity strongly depends on the synthesis protocol and the Pt precursor, which modify the particle size. Higher nitrate rates are achieved using H{sub 2}PtCl{sub 6} than Pt(NH{sub 3}){sub 4}(NO{sub 3}){sub 2}; this is mainly related to the smaller metal particle size of the former, evidenced by HRTEM. Nitrate consumption rate is directly related with the mean particle size. The physical mixture of monometallic catalysts resulted in the highest nitrogen rate.

  13. Polyureas from diamines and carbon dioxide: synthesis, structures and properties.

    Science.gov (United States)

    Wu, Chaoyong; Wang, Jinyao; Chang, Pingjing; Cheng, Haiyang; Yu, Yancun; Wu, Zhijian; Dong, Dewen; Zhao, Fengyu

    2012-01-14

    Polyureas were synthesized from diamines and carbon dioxide in the absence of any catalyst or solvent, analogous to the synthesis of urea from condensation of ammonia with carbon dioxide. The method used carbon dioxide as a carbonyl source to substitute highly toxic isocyanates for the synthesis of polyureas. FTIR and DFT calculations confirmed that strong bidentate hydrogen bonds were formed between urea motifs, and XRD patterns showed that the PUas were highly crystalline and formed a network structure through hydrogen bonds, which served as physical cross-links. The long chain PUas presented a microphase separated morphology as characterized by SAXS and showed a high melting temperature above 200 °C. The PUas showed high resistance to solvents and excellent thermal stability, which benefitted from their special network structures. The PUas synthesized by this method are a new kind of functional material and could serve some areas where their analogues with similar functional groups could not be applied. PMID:22120724

  14. A Simple Synthesis of an N-Doped Carbon ORR Catalyst: Hierarchical Micro/Meso/Macro Porosity and Graphitic Shells.

    Science.gov (United States)

    Eisenberg, David; Stroek, Wowa; Geels, Norbert J; Sandu, Cosmin S; Heller, Adam; Yan, Ning; Rothenberg, Gadi

    2016-01-11

    Replacing platinum as an oxygen reduction catalyst is an important scientific and technological challenge. Herein we report a simple synthesis of a complex carbon with very good oxygen reduction reaction (ORR) activity at pH 13. Pyrolysis of magnesium nitrilotriacetate yields a carbon with hierarchical micro/meso/macro porosity, resulting from in situ templating by spontaneously forming MgO nanoparticles and from etching by pyrolysis gases. The mesopores are lined with highly graphitic shells. The high ORR activity is attributed to a good balance between high specific surface area and mass transport through the hierarchical porosity, and to improved electronic conductivity through the graphitic shells. This novel carbon has a high surface area (1320 m(2) g(-1) ), and high nitrogen content for a single precursor synthesis (∼6 %). Importantly, its synthesis is both cheap and easily scalable.

  15. Polystyrene-supported Phenol/DMAP: an Efficient Binary Catalyst System for CO2 Fixation to Give Cyclic Carbonates

    Institute of Scientific and Technical Information of China (English)

    QI, Chao-Rong; JIANG, Huan-Feng; WANG, Zhao-Yang; ZOU, Bo

    2007-01-01

    Polystyrene-supported phenol (PS-PhOH) was successfully synthesized by alkylation reaction of phenol with 2% DVB cross-linked chloromethylated polystyrene and characterized by IR spectra and elemental analysis. In conjunction with an organic base such as DMAP, DBU, triethylamine (Et3N), diethylamine (Et2NH) or pyridine, the PS-PhOH could effectively catalyze the coupling reaction of carbon dioxide with epoxides to give cyclic carbonates in high yield and selectivity under mild conditions. The binary catalyst system of the PS-PhOH/DMAP was found to be the most active. The influence of reaction temperature, carbon dioxide pressure and reaction time on the yield of product was carefully investigated. The PS-PhOH could be recycled by simple filtration for at least up to ten times without loss of catalytic activity.

  16. Effects of catalyst support and chemical vapor deposition condition on synthesis of multi-walled carbon nanocoils

    Energy Technology Data Exchange (ETDEWEB)

    Suda, Yoshiyuki, E-mail: suda@ee.tut.ac.jp; Iida, Tetsuo; Takikawa, Hirofumi; Harigai, Toru [Department of Electrical and Electronic Information Engineering, Toyohashi University of Technology, Toyohashi, Aichi 441-8580 (Japan); Ue, Hitoshi [Fuji Research Laboratory, Tokai Carbon Co., Ltd., Oyama, Shizuoka 410-1431 (Japan); Umeda, Yoshito [Toho Gas Co., Ltd., Tokai, Aichi 476-8501 (Japan)

    2016-02-01

    Multi-walled carbon nanocoil (MWCNC) is a carbon nanotube (CNT) with helical shape. We have synthesized MWCNCs and MWCNTs hybrid by chemical vapor deposition (CVD). MWCNCs are considered to be a potential material in nanodevices, such as electromagnetic wave absorbers and field emitters. It is very important to take into account the purity of MWCNCs. In this study, we aimed to improve the composition ratio of MWCNCs to MWCNTs by changing catalyst preparation and CVD conditions. As a catalyst, Fe{sub 2}O{sub 3}/zeolite was prepared by dissolving Fe{sub 2}O{sub 3} fine powder and Y-type zeolite (catalyst support material) in ethanol with an Fe density of 0.5wt.% and with a zeolite density of 3.5wt.%. The catalyst-coated Si substrate was transferred immediately onto a hotplate and was heated at 80°C for 5 min. Similarly, Fe{sub 2}O{sub 3}/Al{sub 2}O{sub 3}, Co/zeolite/Al{sub 2}O{sub 3}, Co/zeolite, and Co/Al{sub 2}O{sub 3} were prepared. The effect of the difference of the composite catalysts on synthesis of MWCNCs was considered. The CVD reactor was heated in a tubular furnace to 660-790°C in a nitrogen atmosphere at a flow rate of 1000 ml/min. Subsequently, acetylene was mixed with nitrogen at a flow rate ratio of C{sub 2}H{sub 2}/N{sub 2} = 0.02-0.1. The reaction was kept under these conditions for 10 min. MWCNTs and MWCNCs were well grown by the catalysts of Co/zeolite and Co/Al{sub 2}O{sub 3}. The composition ratio of MWCNCs to MWCNTs was increased by using a combination of zeolite and Al{sub 2}O{sub 3}. The highest composition ratio of MWCNCs to MWCNTs was 12%.

  17. Electrochemical catalyst recovery method

    Science.gov (United States)

    Silva, Laura J.; Bray, Lane A.

    1995-01-01

    A method of recovering catalyst material from latent catalyst material solids includes: a) combining latent catalyst material solids with a liquid acid anolyte solution and a redox material which is soluble in the acid anolyte solution to form a mixture; b) electrochemically oxidizing the redox material within the mixture into a dissolved oxidant, the oxidant having a potential for oxidation which is effectively higher than that of the latent catalyst material; c) reacting the oxidant with the latent catalyst material to oxidize the latent catalyst material into at least one oxidized catalyst species which is soluble within the mixture and to reduce the oxidant back into dissolved redox material; and d) recovering catalyst material from the oxidized catalyst species of the mixture. The invention is expected to be particularly useful in recovering spent catalyst material from petroleum hydroprocessing reaction waste products having adhered sulfides, carbon, hydrocarbons, and undesired metals, and as well as in other industrial applications.

  18. Pt/XC-72 catalysts coated with nitrogen-doped carbon (Pt/XC-72@C–N) for methanol electro-oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Cao, Jun; Chu, Yuanyuan; Tan, Xiaoyao, E-mail: cestanxy@aliyun.com

    2014-03-01

    Pt/XC-72 catalysts coated with N-doped carbon (denoted as Pt/XC-72@C–N) for the electro-oxidation of methanol are prepared through a combined microwave-assisted polyol with in-situ carbonization of N-doped carbon coating process using polyvinylpyrrolidone (PVP), 1-vinyl-3-ethylimidazolium nitrate (VEIN) or 1-ethyl-3-methylimidazolium dicyanamide (EMID) ionic liquid as the N-doped carbon precursor. X-ray diffraction, energy dispersive of X-ray, transmission electron microscopy, X-ray photoelectron spectroscopy, cyclic voltammograms and accelerated aging test techniques are applied to characterize the structure and the electro-catalytic activity of the catalysts. The results show that the Pt particles with the average size of around 2.5 nm are highly dispersed in face-centered cubic crystal structure in the carbon support. The structure of the N-doped carbon coating precursor has considerable influence on the electro-catalytic performance of the catalysts. The resultant catalyst with EMID ionic liquid as the N-doped carbon source exhibits 115.9 m{sup 2} g{sup −1}Pt electrochemical surface area (ESA) and 0.66 A mg{sup −1}Pt catalytic activity towards the electro-oxidation of methanol, which are 1.37 times the ESA and 1.35 times the catalytic activity of the PVP-derived catalyst, and 2.02 times the electrochemical surface area and 1.94 times the catalytic activity of the VEIN-derived catalyst. The appropriate amount of the EMID ionic liquid used in the catalyst synthesis process is around 10 uL for 100 mg XC-72 support so as to obtain the highest electro-catalytic activity. - Highlights: • N-doped carbon coated Pt/C catalyst is prepared for methanol electro-oxidation. • Pt/XC-72@C–N exhibits excellent electrocatalytic activity over uncoated catalysts. • Ionic liquid with anionic cyano groups is most suitable as N-doped carbon precursor. • The appropriate amount of ionic liquid for coating is around 10 μL for 100 mg carbon.

  19. Modulating the morphology and electrical properties of GaAs nanowires via catalyst stabilization by oxygen.

    Science.gov (United States)

    Han, Ning; Yang, Zaixing; Wang, Fengyun; Yip, SenPo; Dong, Guofa; Liang, Xiaoguang; Hung, TakFu; Chen, Yunfa; Ho, Johnny C

    2015-03-11

    Nowadays, III-V compound semiconductor nanowires (NWs) have attracted extensive research interest because of their high carrier mobility favorable for next-generation electronics. However, it is still a great challenge for the large-scale synthesis of III-V NWs with well-controlled and uniform morphology as well as reliable electrical properties, especially on the low-cost noncrystalline substrates for practical utilization. In this study, high-density GaAs NWs with lengths >10 μm and uniform diameter distribution (relative standard deviation σ ∼ 20%) have been successfully prepared by annealing the Au catalyst films (4-12 nm) in air right before GaAs NW growth, which is in distinct contrast to the ones of 2-3 μm length and widely distributed of σ ∼ 20-60% of the conventional NWs grown by the H2-annealed film. This air-annealing process is found to stabilize the Au nanoparticle seeds and to minimize Ostwald ripening during NW growth. Importantly, the obtained GaAs NWs exhibit uniform p-type conductivity when fabricated into NW-arrayed thin-film field-effect transistors (FETs). Moreover, they can be integrated with an n-type InP NW FET into effective complementary metal oxide semiconductor inverters, capable of working at low voltages of 0.5-1.5 V. All of these results explicitly demonstrate the promise of these NW morphology and electrical property controls through the catalyst engineering for next-generation electronics. PMID:25700210

  20. Purification of Carbon Nanotubes Synthesized by Catalytic Decomposition of Methane using Bimetallic Fe-Co Catalysts Supported on MgO

    Energy Technology Data Exchange (ETDEWEB)

    Guan, Beh Hoe; Ramli, Irmawati [Advanced Materials and Nanotechnology Laboratory, Institute of Advanced Technology, Universiti Putra Malaysia 43400 UPM Serdang, Selangor (Malaysia); Yahya, Noorhana [Fundamental and Applied Science Department Universiti Teknologi Petronas, Bandar Seri Iskandar, 31750 Tronoh, Perak (Malaysia); Pah, Lim Kean, E-mail: irmawati@science.upm.edu.my [Physics department, Faculty of Science, Universiti Putra Malaysia 43400 UPM Serdang, Selangor (Malaysia)

    2011-02-15

    This work reports the synthesis of carbon nanotubes by catalytic decomposition of methane using bimetallic Fe-Co catalysts supported on MgO. Transmission electron microscopy (TEM) results show the as-prepared carbon nanotubes are multi-walled carbon nanotubes (MWCNTs) with diameter in the range of 15nm to 45nm. Purification of as-prepared MWCNTs was carried out by acid and heat treatment method. EDX results show the Fe, Co and MgO catalysts were successfully removed by refluxing the as-prepared MWCNTs in 3M H{sub 2}SO{sub 4}.