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Sample records for activated carbon catalysts

  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. Preparation And Characterization Of Cr/Activated Carbon Catalyst From Palm Empty Fruit Bunch

    Directory of Open Access Journals (Sweden)

    Zainal Fanani

    2016-02-01

    Full Text Available Preparation and characterization of Cr/activated carbon catalyst from palm empty fruit bunch had been done. The research were to determine the effect of carbonization temperature towards adsorption of ammonia, iodine number, metilen blue number, and porosity of activated carbon and Cr/activated carbon catalyst. The determination of porosity include surface area, micropore volume and total pore volume. The results showed the best carbonization temperature activated carbon and Cr/activated carbon catalyst at 700°C. The adsorption ammonia of activated carbon and Cr/activated carbon catalyst as 6.379 mmol/g and 8.1624 mmol/g. The iodine number of activated carbon and Cr/activated carbon catalyst as 1520.16 mg/g and 1535.67 mg/g. The metilen blue number of activated carbon and Cr/activated carbon catalyst as 281.71 mg/g and 319.18 mg/g. The surface area of activated carbon and Cr/activated carbon catalyst as 1527.80 m2/g and 1652.58 m2/g. The micropore volume of activated carbon and Cr/activated carbon catalyst as 0.7460 cm3/g and 0.8670 cm3/g. The total pore volume of activated carbon and Cr/activated carbon catalyst as 0.8243 cm3/g and 0.8970 cm3/g.

  3. 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.

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

    International Nuclear Information System (INIS)

    Zulkarnain Zainal; Chan, Sook Keng; Abdul Halim Abdullah

    2008-01-01

    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 TiO 2 / AC was found to be two times better than the removal by immobilised AC or immobilised TiO 2 alone. In 4 hours and with the concentration of 10 ppm, TiO 2 loaded activated carbon prepared from 1.5 g/ 15.0 mL suspension produced 99.50 % dye removal. (author)

  5. Highly active carbon supported Pd cathode catalysts for direct formic acid fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Mikolajczuk-Zychora, A., E-mail: amikolajczuk@ichf.edu.pl [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland); Borodzinski, A.; Kedzierzawski, P.; Mierzwa, B. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland); Mazurkiewicz-Pawlicka, M. [Faculty of Materials Science and Engineering, Warsaw University of Technology, Wołoska 141, 02-507 Warsaw (Poland); Faculty of Chemical and Process Engineering, Warsaw University of Technology, Warynskiego 1, Warsaw (Poland); Stobinski, L. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland); Faculty of Chemical and Process Engineering, Warsaw University of Technology, Warynskiego 1, Warsaw (Poland); Ciecierska, E. [Faculty of Materials Science and Engineering, Warsaw University of Technology, Wołoska 141, 02-507 Warsaw (Poland); Zimoch, A.; Opałło, M. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw (Poland)

    2016-12-01

    Highlights: • Palladium catalyst used on the cathode DFAFC is comparable to commercial platinum catalyst. • The treatment of carbon supports in nitric acid(V) increases the electrochemically available metal surface area and the catalytic activity in oxygen reduction reaction of catalysts. - Abstract: One of the drawbacks of low-temperature fuel cells is high price of platinum-based catalysts used for the electroreduction of oxygen at the cathode of the fuel cell. The aim of this work is to develop the palladium catalyst that will replace commonly used platinum cathode catalysts. A series of palladium catalysts for oxygen reduction reaction (ORR) were prepared and tested on the cathode of Direct Formic Acid Fuel Cell (DFAFC). Palladium nanoparticles were deposited on the carbon black (Vulcan) and on multiwall carbon nanotubes (MWCNTs) surface by reduction of palladium(II) acetate dissolved in ethanol. Hydrazine was used as a reducing agent. The effect of functionalization of the carbon supports on the catalysts physicochemical properties and the ORR catalytic activity on the cathode of DFAFC was studied. The supports were functionalized by treatment in nitric acid for 4 h at 80 °C. The structure of the prepared catalysts has been characterized by thermogravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscope (TEM) and cyclic voltammetry (CV). Hydrophilicity of the catalytic layers was determined by measuring contact angles of water droplets. The performance of the prepared catalysts has been compared with that of the commercial 20 wt.% Pt/C (Premetek) catalyst. The maximum power density obtained for the best palladium catalyst, deposited on the surface of functionalized carbon black, is the same as that for the commercial Pt/C (Premetek). Palladium is cheaper than platinum, therefore the developed cathode catalyst is promising for future applications.

  6. Highly active carbon supported Pd cathode catalysts for direct formic acid fuel cells

    Science.gov (United States)

    Mikolajczuk-Zychora, A.; Borodzinski, A.; Kedzierzawski, P.; Mierzwa, B.; Mazurkiewicz-Pawlicka, M.; Stobinski, L.; Ciecierska, E.; Zimoch, A.; Opałło, M.

    2016-12-01

    One of the drawbacks of low-temperature fuel cells is high price of platinum-based catalysts used for the electroreduction of oxygen at the cathode of the fuel cell. The aim of this work is to develop the palladium catalyst that will replace commonly used platinum cathode catalysts. A series of palladium catalysts for oxygen reduction reaction (ORR) were prepared and tested on the cathode of Direct Formic Acid Fuel Cell (DFAFC). Palladium nanoparticles were deposited on the carbon black (Vulcan) and on multiwall carbon nanotubes (MWCNTs) surface by reduction of palladium(II) acetate dissolved in ethanol. Hydrazine was used as a reducing agent. The effect of functionalization of the carbon supports on the catalysts physicochemical properties and the ORR catalytic activity on the cathode of DFAFC was studied. The supports were functionalized by treatment in nitric acid for 4 h at 80 °C. The structure of the prepared catalysts has been characterized by thermogravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscope (TEM) and cyclic voltammetry (CV). Hydrophilicity of the catalytic layers was determined by measuring contact angles of water droplets. The performance of the prepared catalysts has been compared with that of the commercial 20 wt.% Pt/C (Premetek) catalyst. The maximum power density obtained for the best palladium catalyst, deposited on the surface of functionalized carbon black, is the same as that for the commercial Pt/C (Premetek). Palladium is cheaper than platinum, therefore the developed cathode catalyst is promising for future applications.

  7. Carbons and carbon supported catalysts in hydroprocessing

    Energy Technology Data Exchange (ETDEWEB)

    Furimsky, Edward

    2009-07-01

    This book is a comprehensive summary of recent research in the field and covers all areas of carbons and carbon materials. The potential application of carbon supports, particularly those of carbon black (CB) and activated carbon (AC) in hydroprocessing catalysis are covered. Novel carbon materials such as carbon fibers and carbon nano tubes (CNT) are also covered, including the more recent developments in the use of fullerenes in hydroprocessing applications. Although the primary focus of this book is on carbons and carbon supported catalysts, it also identifies the difference in the effect of carbon supports compared with the oxidic supports, particularly that of the Al{sub 2}O{sub 3}. The difference in catalyst activity and stability was estimated using both model compounds and real feeds under variable conditions. The conditions applied during the preparation of carbon supported catalysts are also comprehensively covered and include various methods of pretreatment of carbon supports to enhance catalyst performance. The model compounds results consistently show higher hydrodesulfurization and hydrodeoxygenation activities of carbon supported catalysts than that of the Al{sub 2}O{sub 3} supported catalysts. Also, the deactivation of the former catalysts by coke deposition was much less evident. Chapter 6.3.1.3 is on carbon-supported catalysts: coal-derived liquids.

  8. Effects of Activated Carbon Surface Property on Structure and Activity of Ru/AC Catalysts

    Science.gov (United States)

    Xu, S. K.; Li, L. M.; Guo, N. N.

    2018-05-01

    The activated carbon (AC) was modified by supercritical (SC) methanol, HNO3 oxidation, or HNO3 oxidation plus SC methanol, respectively. Then, the original and the modified AC were used as supports for Ru/AC catalysts prepared via the impregnation method. The results showed that the SC methanol modification decreased the content of surface acidic groups of AC. While HNO3 oxidation displayed the opposite behavior. Furthermore, the dispersion of ruthenium and the activity of catalysts were highly dependent on the content of surface acidic groups, and the SC methanol modified sample exhibited the highest activity for hydrogenation of glucose.

  9. Activity of Cu-activated carbon fiber catalyst in wet oxidation of ammonia solution.

    Science.gov (United States)

    Hung, Chang-Mao

    2009-07-30

    Aqueous solutions of 200-1000 mg/L of ammonia were oxidized in a trickle-bed reactor using Cu-activated carbon fiber (ACF) catalysts, which were prepared by incipient wet impregnation with aqueous solutions of copper nitrate that was deposited on ACF substrates. The results reveal that the conversion of ammonia by wet oxidation in the presence of Cu-ACF catalysts was a function of the metal loading weight ratio of the catalyst. The total conversion efficiency of ammonia was 95% during wet oxidation over the catalyst at 463 K at an oxygen partial pressure of 3.0 MPa. Moreover, the effect of the initial concentration of ammonia and the reaction temperature on the removal of ammonia from the effluent streams was also studied at a liquid space velocity of less than 3.0 h(-1).

  10. Activity of Cu-activated carbon fiber catalyst in wet oxidation of ammonia solution

    Energy Technology Data Exchange (ETDEWEB)

    Hung, Chang-Mao, E-mail: hungcm1031@gmail.com [Department of Industry Engineering and Management, Yung-Ta Institute of Technology and Commerce, 316 Chung-shan Road, Linlo, Pingtung 909, Taiwan (China)

    2009-07-30

    Aqueous solutions of 200-1000 mg/L of ammonia were oxidized in a trickle-bed reactor using Cu-activated carbon fiber (ACF) catalysts, which were prepared by incipient wet impregnation with aqueous solutions of copper nitrate that was deposited on ACF substrates. The results reveal that the conversion of ammonia by wet oxidation in the presence of Cu-ACF catalysts was a function of the metal loading weight ratio of the catalyst. The total conversion efficiency of ammonia was 95% during wet oxidation over the catalyst at 463 K at an oxygen partial pressure of 3.0 MPa. Moreover, the effect of the initial concentration of ammonia and the reaction temperature on the removal of ammonia from the effluent streams was also studied at a liquid space velocity of less than 3.0 h{sup -1}.

  11. Activity of Cu-activated carbon fiber catalyst in wet oxidation of ammonia solution

    International Nuclear Information System (INIS)

    Hung, Chang-Mao

    2009-01-01

    Aqueous solutions of 200-1000 mg/L of ammonia were oxidized in a trickle-bed reactor using Cu-activated carbon fiber (ACF) catalysts, which were prepared by incipient wet impregnation with aqueous solutions of copper nitrate that was deposited on ACF substrates. The results reveal that the conversion of ammonia by wet oxidation in the presence of Cu-ACF catalysts was a function of the metal loading weight ratio of the catalyst. The total conversion efficiency of ammonia was 95% during wet oxidation over the catalyst at 463 K at an oxygen partial pressure of 3.0 MPa. Moreover, the effect of the initial concentration of ammonia and the reaction temperature on the removal of ammonia from the effluent streams was also studied at a liquid space velocity of less than 3.0 h -1 .

  12. Process intensification by combination of activated carbon supported catalysts and alternative energy sources

    OpenAIRE

    Calvino Casilda, Vanesa; Pérez-Mayoral, E.

    2014-01-01

    [EN] Activated carbons are well known for their catalytic properties and for being used as a catalyst support in heterogeneous catalysis. Activated carbons possess most of the desired properties of a catalyst support; inertness towards unwanted reactions, stability under regeneration and reaction conditions, suitable mechanical properties, tunable surface area, porosity, and the possibility of being manufactured in different size and shape. On the other hand, the in...

  13. Engineering catalytic activity via ion beam bombardment of catalyst supports for vertically aligned carbon nanotube growth

    Science.gov (United States)

    Islam, A. E.; Nikolaev, P.; Amama, P. B.; Zakharov, D.; Sargent, G.; Saber, S.; Huffman, D.; Erford, M.; Semiatin, S. L.; Stach, E. A.; Maruyama, B.

    2015-09-01

    Carbon nanotube growth depends on the catalytic activity of metal nanoparticles on alumina or silica supports. The control on catalytic activity is generally achieved by variations in water concentration, carbon feed, and sample placement on a few types of alumina or silica catalyst supports obtained via thin film deposition. We have recently expanded the choice of catalyst supports by engineering inactive substrates like c-cut sapphire via ion beam bombardment. The deterministic control on the structure and chemistry of catalyst supports obtained by tuning the degree of beam-induced damage have enabled better regulation of the activity of Fe catalysts only in the ion beam bombarded areas and hence enabled controllable super growth of carbon nanotubes. A wide range of surface characterization techniques were used to monitor the catalytically active surface engineered via ion beam bombardment. The proposed method offers a versatile way to control carbon nanotube growth in patterned areas and also enhances the current understanding of the growth process. With the right choice of water concentration, carbon feed and sample placement, engineered catalyst supports may extend the carbon nanotube growth yield to a level that is even higher than the ones reported here, and thus offers promising applications of carbon nanotubes in electronics, heat exchanger, and energy storage.

  14. Application in industry and energy production of active carbon/cobalt catalyst for nitrogen oxide neutralization

    International Nuclear Information System (INIS)

    Mekhandzhiev, D.; Nikolov, R.; Lyutskanov, L.; Dushanov, D.; Lakov, L.

    1997-01-01

    A new material for neutralization of nitrogen oxides is presented. Two or three metals containing catalysts with a good activity and selectivity towards NO x have been obtained. Preparation of carbon catalysts by deposition of the active phase precursor on the initial carbon material prior to activation is considered as the most promising method. An active carbon-based catalyst (AC/Co) has been synthesized Apricot shells preliminary impregnated with a water-alcohol solution of Co nitrate have been used as initial carbon material. after drying they have been subjected to one-phase steam pyrolysis using a fix-bed reactor. The catalyst thus obtained has a specific surface area (BET) of 53 m 2 g -1 , a favorable mesopore volume/total volume ratio (about 0.85) determined by nitrogen adsorption, a suitable mesopore distribution, about 70% of the mesopores being characterized by r p larger than 25 A and a high dispersion of the Co oxide phase. In addition the catalyst possesses the necessary mechanical resistance. The catalyst has exhibited a high activity with respect to NO x reduction with CO at low temperatures (at 150-250 o C which are the temperatures of industrial flue gases, nO conversion up to 60-95% occurs) and a high selectivity. No presence of H 2 O has been established over the whole temperature range (100-300 o C). An additional advantage of the catalyst is the fact that the amount of CO above 150 o C is lower than the stoichiometric which indicates parallel participation in the process of both the active phase and the support (active carbon) It is also important that the presented catalyst has a low price due to the use of waste products from agriculture and the elimination of special thermal treatment of the supported Co nitrate. There are possibilities of using of other organic wastes from agriculture as well as wastes obtained during flotation of coal. (author)

  15. Trickle bed reactor for the oxidation of phenol over active carbon catalyst

    OpenAIRE

    Gabbiye, Nigus; Font Capafons, Josep; Fortuny Sanromá, Agustín; Bengoa, Christophe José; Fabregat Llangotera, Azael; Stüber, Frank Erich

    2009-01-01

    The catalytic wet air oxidation of phenol using activated carbon has been performed in a laboratory trickle bed reactor over a wide range of operating variables (PO2, T, FL and Cph,o) and hydrodynamic conditions. The influence of different start-up procedures (saturation of activated carbon) has also been tested. Further improvement of activity and stability has been checked for by using dynamic TBR operation concept or impregnated Fe/carbon catalyst. The results obtained confi...

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

    KAUST Repository

    Shuai, Danmeng; Choe, Jong Kwon; Shapley, John R.; Werth, Charles J.

    2012-01-01

    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.

  17. 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.

  18. Catalytic performance of activated carbon supported cobalt catalyst for CO2 reforming of CH4.

    Science.gov (United States)

    Zhang, Guojie; Su, Aiting; Du, Yannian; Qu, Jiangwen; Xu, Ying

    2014-11-01

    Syngas production by CO2 reforming of CH4 in a fixed bed reactor was investigated over a series of activated carbon (AC) supported Co catalysts as a function of Co loading (between 15 and 30wt.%) and calcination temperature (Tc=300, 400 or 500°C). The catalytic performance was assessed through CH4 and CO2 conversions and long-term stability. XRD and SEM were used to characterize the catalysts. It was found that the stability of Co/AC catalysts was strongly dependent on the Co loading and calcination temperature. For the loadings (25wt.% for Tc=300°C), stable activities have been achieved. The loading of excess Co (>wt.% 25) causes negative effects not only on the performance of the catalysts but also on the support surface properties. In addition, the experiment showed that ultrasound can enhance and promote dispersion of the active metal on the carrier, thus improving the catalytic performance of the catalyst. The catalyst activity can be long-term stably maintained, and no obvious deactivation has been observed in the first 2700min. After analyzing the characteristics, a reaction mechanism for CO2 reforming of CH4 over Co/AC catalyst was proposed. Copyright © 2014 Elsevier Inc. All rights reserved.

  19. Anti-bacteria activity of carbon nanotubes grown on trimetallic catalyst

    Science.gov (United States)

    Ibrahim, S. O.; Abdulkareem, A. S.; Isah, K. U.; Ahmadu, U.; Bankole, M. T.; Kariim, I.

    2018-06-01

    Trimetallic catalyst was prepared using wet impregnation method to produce carbon nanotubes (CNTs) through the method of catalytic chemical vapor deposition (CCVD). Characterization of the developed catalyst and CNTs were carried out using thermogravimetric analysis (TGA), x-ray diffraction (XRD), specific surface area Brunauer-Emmett-Teller (BET), Fourier-transform infrared spectroscopy (FTIR), high-resolution scanning electron microscopy (HRSEM)/energy dispersive x-ray spectroscopy (EDS) and high-resolution transmission electron microscopy (HRTEM)/selected area electron diffraction (SAED). The BET and TGA analysis indicated that the catalyst has a high surface area and is thermally stable. The FTIR of the developed catalyst shows notable functional group with presence of unbound water. The HRSEM of the catalyst revealed agglomerated, homogeneous and porous particles while the HRSEM/HRTEM of the produced CNTs gave the formation of long strand of multiwalled carbon nanotubes (MWCNTs), and homogeneous crystalline fringe like structure with irregular diameter. EDS revealed the dominance of carbon in the elemental composition. XRD/SAED patterns of the catalyst suggest high dispersion of the metallic particles in the catalyst mixture while that of the CNTs confirmed that the produced MWCNTs were highly graphitized and crystalline in nature with little structural defects. The anti-bacteria activity of the produced MWCNTs on Klebsiella pneumoneae, Escherichia coli, and Pseudomonas aeruginosa was also carried out. It was observed that the produced MWCNTs have an inhibitory property on bacteria; Escherichia coli and Klebsiella pneumoneae from zero day ( and ) through to twelfth day (Nil count) respectively. It has no effect on Pseudomonas aeruginosa with too numerous to count at zero-sixth day, but a breakdown in its growth at ninth-twelfth day (). This study implied that MWCNTs with varying diameter and well-ordered nano-structure can be produced from catalyst via CCVD

  20. Immersion Calorimetry for the Characterization of PD Catalysts Supported on Activated Carbon

    Directory of Open Access Journals (Sweden)

    Liliana Giraldo

    2009-01-01

    Full Text Available Activated carbons obtained from coconut peel were oxidized using hydrogen peroxide. Superficial characteristics of these carbons were determined through N2 and CO2 isotherms and functional groups were characterized by TPD. Finally, the microcalorimetry technique was used in order to obtain the immersion enthalpies in diverse liquids and established the relation between them and the results obtained by the other characterization techniques. The results suggested that the immersion calorimetry allow establishing the difference between the supports and the catalysts.

  1. Novel synthesis of highly durable and active Pt catalyst encapsulated in nitrogen containing carbon for polymer electrolyte membrane fuel cell

    Science.gov (United States)

    Lee, Hyunjoon; Sung, Yung-Eun; Choi, Insoo; Lim, Taeho; Kwon, Oh Joong

    2017-09-01

    Novel synthesis of a Pt catalyst encapsulated in a N-containing carbon layer for use in a polymer electrolyte membrane fuel cell is described in this study. A Pt-aniline complex, formed by mixing Pt precursor and aniline monomer, was used as the source of Pt, C, and N. Heat treatment of the Pt-aniline complex with carbon black yielded 5 nm Pt nanoparticles encapsulated by a N-containing carbon layer originating from aniline carbonization. The synthesized Pt catalyst exhibited higher mass specific activity to oxygen reduction reaction than that shown by conventional Pt/C catalyst because pyridinic N with graphitic carbon in the carbon layer provided active sites for oxygen reduction reaction in addition to those provided by Pt. In single cell testing, initial performance of the synthesized catalyst was limited because the thick catalyst layer increased resistance related to mass transfer. However, it was observed that the carbon layer successfully prevented Pt nanoparticles from growing via agglomeration and Ostwald ripening under fuel cell operation, thereby improving durability. Furthermore, a mass specific performance of the synthesized catalyst higher than that of a conventional Pt/C catalyst was achieved by modifying the synthesized catalyst's layer thickness.

  2. Improved hydrogen generation from alkaline NaBH{sub 4} solution using cobalt catalysts supported on modified activated carbon

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Dongyan; Guo, Qingjie; Yue, Xuehai [College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042 (China); Dai, Ping [College of Electromechanical Engineering, Qingdao University of Science and Technology, Qingdao 266061 (China)

    2008-12-15

    Hydrogen production from alkaline sodium borohydride (NaBH{sub 4}) solution via hydrolysis process over activated carbon supported cobalt catalysts is studied. Activated carbons are used in their original form and after liquid phase oxidation with HNO{sub 3}. The changes in surface functional groups of the activated carbon are detected by FTIR spectroscopy. The effects of HNO{sub 3} oxidation on the properties of the activated carbon and the resulting catalyst performance are investigated. FTIR analysis reveals that the oxidative treatment leads to the formation of various functional groups on the surface of the activated carbon. Cobalt catalysts supported on the modified activated carbon are found to exhibit higher activity and stability. (author)

  3. Activated carbon derived from chitosan as air cathode catalyst for high performance in microbial fuel cells

    Science.gov (United States)

    Liu, Yi; Zhao, Yong; Li, Kexun; Wang, Zhong; Tian, Pei; Liu, Di; Yang, Tingting; Wang, Junjie

    2018-02-01

    Chitosan with rich of nitrogen is used as carbon precursor to synthesis activated carbon through directly heating method in this study. The obtained carbon is activated by different amount of KOH at different temperatures, and then prepared as air cathodes for microbial fuel cells. Carbon sample treated with double amount of KOH at 850 °C exhibits maximum power density (1435 ± 46 mW m-2), 1.01 times improved, which ascribes to the highest total surface area, moderate micropore and mesoporous structure and the introduction of nitrogen. The electrochemical impedance spectroscopy and powder resistivity state that carbon treated with double amount of KOH at 850 °C possesses lower resistance. The other electrochemical measurements demonstrate that the best kinetic activity make the above treated sample to show the best oxygen reduction reaction activity. Besides, the degree of graphitization of samples increases with the activated temperature increasing, which is tested by Raman. According to elemental analysis and X-ray photoelectron spectroscopy, all chitosan samples are nitrogen-doped carbon, and high content nitrogen (pyridinic-N) improves the electrochemical activity of carbon treated with KOH at 850 °C. Thus, carbon materials derived from chitosan would be an optimized catalyst for oxygen reduction reaction in microbial fuel cell.

  4. Structure-activity relationships of carbon-supported platinum-bismuth and platinum-antimony oxidation catalysts

    CSIR Research Space (South Africa)

    Maphoru, MV

    2017-04-01

    Full Text Available Compositional and morphological studies on supported platinum are important for the improvement and expanded use of catalysts for oxidative coupling reactions. Nanocomposites consisting of 5% Pt supported on activated carbon and promoted with 5% Bi...

  5. 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.

  6. Synthesis of carbonate esters by carboxymethylation using NaAlO2 as a highly active heterogeneous catalyst

    OpenAIRE

    Ramesh, Sreerangappa; Indukuri, Kiran; Riant, Olivier; Debecker, Damien

    2018-01-01

    Sodium aluminate is presented as a highly active heterogeneous catalyst able to convert a range of alcohols into the corresponding mixed carbonate esters, in high yield and under green conditions. The reaction is carried out using dimethyl carbonate both as a reactant and solvent, at 90°C. Allylic, aliphatic and aromatic alcohols are converted in good yields. The solid catalyst is shown to be truly heterogeneous, resistant to leaching, and recyclable.

  7. Esterification of fatty acids using sulfated zirconia and composites activated carbon/sulfated zirconia catalysts

    International Nuclear Information System (INIS)

    Brum, Sarah S.; Santos, Valeria C. dos; Destro, Priscila; Guerreiro, Mario Cesar

    2011-01-01

    In this work sulfated zirconia (SZr) and activated carbon/SZr composites produced by impregnation method with or without heating treatment step (CABC/SZr-I and CABC/SZr-I SC) and by the method of synthesis of SZr on the carbon (CABC/SZr-S) was used as catalysts in the esterification reactions of fatty acids. The SZr presented very active, conversions higher than 90% were obtained after 2 h of reaction. The activity of the composite CABC/SZr-I20%SC was up to 92%, however, this was directly related to time and temperature reactions. CABC/SZr-I and CABC/SZr-S were less active in esterification reactions, what could be attributed to its low acidity. (author)

  8. Preparation of a Carbon-Based Solid Acid Catalyst by Sulfonating Activated Carbon in a Chemical Reduction Process

    Directory of Open Access Journals (Sweden)

    Xiao-Yan Liu

    2010-10-01

    Full Text Available Sulfonated (SO3H-bearing activated carbon (AC-SO3H was synthesized by an aryl diazonium salt reduction process. The obtained material had a SO3H density of 0.64 mmol·g-1 and a specific surface area of 602 m2·g-1. The catalytic properties of AC-SO3H were compared with that of two commercial solid acid catalysts, Nafion NR50 and Amberlyst-15. In a 10-h esterification reaction of acetic acid with ethanol, the acid conversion with AC-SO3H (78% was lower than that of Amberlyst-15 (86%, which could be attributed to the fact that the SO3H density of the sulfonated carbon was lower than that of Amberlyst-15 (4.60 mmol·g-1. However, AC-SO3H exhibited comparable and even much higher catalytic activities than the commercial catalysts in the esterification of aliphatic acids with longer carbon chains such as hexanoic acid and decanoic acid, which may be due to the large specific surface area and mesoporous structures of the activated carbon. The disadvantage of AC-SO3H is the leaching of SO3H group during the reactions.

  9. Electrocatalytic activity of carbon-supported catalysts for direct ethanol fuel cell applications

    Energy Technology Data Exchange (ETDEWEB)

    Rodriguez Varela, F.J. [CINVESTAV-Unidad Saltillo, Coahuila, (Mexico). Grupo de Investigacion en Energia; Savadogo, O. [Ecole Polytechnique de Montreal, Montreal, PQ (Canada). Laboratoire de nouveaux materiaux pour l' energie et l' electrochimie

    2008-07-01

    Proton exchange membrane fuel cells (PEMFCs) can be fueled with hydrogen, alcohols, hydrocarbons and acetals. Ethanol is an important fuel candidate because it can be electro-oxidized to carbon dioxide on platinum (Pt)-based electrocatalysts in a direct ethanol fuel cell (DEFC) at relatively low temperatures. This study investigated the electrocatalytic activity of some carbon-supported electrocatalysts towards the ethanol oxidation (EOR) and the oxygen reduction reaction (ORR) in the presence of ethanol. Compared to other anode catalysts such as Pt, PtRu and Pt oxide, anodes based on PtSn alloys have a higher catalytic activity for the EOR. When tested in a DEFC, the current density at 0.4V and 90 degrees C based on a PtSn/C anode and a Pt/C cathode was 2 times higher than that of a cell based on a PtRu/C-Pt/C membrane electrode assembly (MEA) configuration. In addition, cathode catalysts based on Ru/C had good catalytic activity for the ORR and exhibited high selectivity for this reaction in the presence of ethanol. The results showed that in the presence of 0.125, 0.25 or 0.5 M ethanol concentrations, a decrease in onset potential of about 60, 62 and 68 mV emerged, respectively. These values were about 10 times lower than those measured for some Pt-based cathode catalysts tested in this study in the presence of 0.125 M EtOH. 20 refs., 5 figs.

  10. Selective adsorption of refractory sulfur species on active carbons and carbon based CoMo catalyst.

    Science.gov (United States)

    Farag, Hamdy

    2007-03-01

    Adsorption technique could be a reliable alternative in removing to a certain remarkable extent the sulfur species from the feedstock of petroleum oil. The performance of various carbons on adsorption of model sulfur compounds in a simulated feed solution and the sulfur containing compounds in the real gas oil was evaluated. The adsorption experiments have been carried out in a batch scale at ambient temperature and under the atmospheric pressure. In general, the most refractory sulfur compounds in the hydrotreatment reactions were selectively removed and adsorbed. It was found that the adsorbents affinities to dibenzothiophene and 4,6-dimethyldibenzothiophene were much more favored and pronounced than the aromatic matrices like fluorene, 1-methylnaphthalene and 9-methylanthracene. Among the sulfur species, 4,6-dimethyldibenzothiophene was the highest to be removed in terms of both selectivity and capacity over all the present adsorbents. The studied adsorbents showed significant capacities for the polyaromatic thiophenes. The electronic characteristics seem to play a certain role in such behavior. Regeneration of the used adsorbent was successfully attained either by washing it with toluene or by the release of the adsorbates through heat treatment. A suggested adsorptive removal process of sulfur compounds from petroleum distillate over carbon supported CoMo catalyst was discussed.

  11. Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts.

    Science.gov (United States)

    Mistry, Hemma; Choi, Yong-Wook; Bagger, Alexander; Scholten, Fabian; Bonifacio, Cecile S; Sinev, Ilya; Divins, Nuria J; Zegkinoglou, Ioannis; Jeon, Hyo Sang; Kisslinger, Kim; Stach, Eric A; Yang, Judith C; Rossmeisl, Jan; Roldan Cuenya, Beatriz

    2017-09-11

    Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO 2 is to become a viable route to the synthesis of industrial feedstocks and fuels. A plasma oxidation pre-treatment of silver foil enhances the number of low-coordinated catalytically active sites, which dramatically lowers the overpotential and increases the activity of CO 2 electroreduction to CO. At -0.6 V versus RHE more than 90 % Faradaic efficiency towards CO was achieved on a pre-oxidized silver foil. While transmission electron microscopy (TEM) and operando X-ray absorption spectroscopy showed that oxygen species can survive in the bulk of the catalyst during the reaction, quasi in situ X-ray photoelectron spectroscopy showed that the surface is metallic under reaction conditions. DFT calculations reveal that the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields drastically decrease the overpotential of CO 2 electroreduction. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Influence of plasma treatment of carbon blacks on electrochemical activity of Pt/carbon blacks catalysts for DMFCs

    Science.gov (United States)

    Kim, Seok; Cho, Mi-Hwa; Lee, Jae-Rock; Park, Soo-Jin

    In this work, in order to improve the dispersion of platinum catalysts deposited on carbon materials, the effects of surface plasma treatment of carbon blacks (CBs) were investigated. The surface characteristics of the CBs were determined by fourier transformed-infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), and Boehm's titration method. The electrochemical properties of the plasma-treated CBs-supported Pt (Pt/CBs) catalysts were analyzed by linear sweep voltammetry (LSV) experiments. From the results of FT-IR and acid-base values, N 2-plasma treatment of the CBs at 300 W intensity led to a formation of a free radical on the CBs. The peak intensity increased with increase of the treatment time, due to the formation of new basic functional groups (such as C-N, C dbnd N, -NH 3 +, -NH, and dbnd NH) by the free radical on the CBs. Accordingly, the basic values were enhanced by the basic functional groups. However, after a specific reaction time, N 2-plasma treatment could hardly influence on change of the surface functional groups of CBs, due to the disappearance of free radical. Consequently, it was found that optimal treatment time was 30 s for the best electro activity of Pt/CBs catalysts and the N 2-plasma treated Pt/CBs possessed the better electrochemical properties than the pristine Pt/CBs.

  13. Pt Nanostructures/N-Doped Carbon hybrid, an Efficient Catalyst for Hydrogen Evolution/Oxidation Reactions: Enhancing its Base Media Activity through Bifunctionality of the Catalyst.

    Science.gov (United States)

    Barman, Sudip; Kundu, Manas; Bhowmik, Tanmay; Mishra, Ranjit

    2018-06-04

    Design and synthesis of active catalyst for HER/HOR are important for the development of hydrogen based renewable technologies. We report synthesis of Pt nanostructures-N-doped carbon hybrid (Pt-(PtO2)-NSs/C) for HER/HOR applications. The HER activity of this Pt-(PtOx)-NSs/C catalyst is 4 and 6.5 times better than commercial Pt/C in acid and base. The catalyst exhibits a current density of 10 mA/cm2 at overpotentials of 5 and 51 mV with tafel slopes of 29 and 64mV/dec in in 0.5 M H2SO4 and 0.5 M KOH. This catalyst also showed superior HOR activity at all pH values. The HER/HOR activity of Pt-(PtOx)-NSs/C and PtOx-free Pt-Nanostructures/C (PtNSs/C) catalysts are comparable in acid. The presence of PtOx in Pt-(PtOx)-NSs/C makes this Pt-catalyst more HER/HOR active in base media. The activity of Pt-(PtOx)NSs/C catalyst is 5 fold higher than that of PtNSs/C catalyst in basic medium although their activity is comparable in acid. Hydrogen binding energy and oxophilicity are the two equivalent descriptors for HER/HOR in basic media. We propose a bi-functional mechanism for the enhanced alkaline HER/HOR activity of Pt(PtOx)-NSs/C catalyst. In bi-functional Pt-(PtOx)-NSs/C catalyst, PtOx provide an active site for OH- adsorption to form OHads which reacts with hydrogen intermediate (Hads), present at neighbouring Pt sites to form H2O leading to enhancement of HOR activity in basic medium This work may provide opportunity to develop catalysts for various renewable energy technologies. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. Hydrogen storage of catalyst-containing activated carbon fibers and effect of surface modification

    International Nuclear Information System (INIS)

    Ikpyo Hong; Seong Young Lee; Kyung Hee Lee; Sei Min Park

    2005-01-01

    Introduction: The hydrogen storage capacities of many kind of carbon nano materials have been reported with possibility and improbability. It is reported that specific surface area of carbon nano material has not a close relation to hydrogen storage capacity. This result shows that there is difference between specific surface area measured by isothermal nitrogen adsorption and direct measurement of adsorption with hydrogen and suggests that the carbon material with relatively low specific surface area can have high hydrogen storage capacity when they have effective nano pore. In this study, petroleum based isotropic pitch was hybridized with several kinds of transitional metal base organometallic compound solved with organic solvent and spun by electro-spinning method. The catalyst-dispersed ACFs were prepared and characterized and hydrogen storage capacity was measured. The effect of surface modification of ACFs by physical and chemical treatment was also investigated. Experimental: The isotropic precursor pitch prepared by nitrogen blowing from naphtha cracking bottom oil was hybridized with transitional metal based acetyl acetonates and spun by solvent electro-spinning. Tetrahydrofuran and quinoline were used as solvent with various mixing ratio. High voltage DC power generator which could adjust in the range of 0-60000 V and 2 mA maximum current was used to supply electrostatic force. At the solvent electro-spinning, solvent mixing ratio and pitch concentration, voltage and spinning distance were varied and their influences were investigated. The catalyst-dispersed electro-spun pitch fibers were thermal stabilized, carbonized and activated by conventional heat treatment for activated carbon fiber. Prepared fibers were observed by high resolution SEM and pore properties were characterized by Micromeritics ASAP2020 model physi-sorption analyzer. Hydrogen storage capacities were measured by equipment modified from Thermo Cahn TherMax 500 model high pressure

  15. A New Energy-Saving Catalytic System: Carbon Dioxide Activation by a Metal/Carbon Catalyst.

    Science.gov (United States)

    Yun, Danim; Park, Dae Sung; Lee, Kyung Rok; Yun, Yang Sik; Kim, Tae Yong; Park, Hongseok; Lee, Hyunjoo; Yi, Jongheop

    2017-09-22

    The conversion of CO 2 into useful chemicals is an attractive method to reduce greenhouse gas emissions and to produce sustainable chemicals. However, the thermodynamic stability of CO 2 means that a lot of energy is required for its conversion into chemicals. Here, we suggest a new catalytic system with an alternative heating system that allows minimal energy consumption during CO 2 conversion. In this system, electrical energy is transferred as heat energy to the carbon-supported metal catalyst. Fast ramping rates allow high operating temperatures (T app =250 °C) to be reached within 5 min, which leads to an 80-fold decrease of energy consumption in methane reforming using CO 2 (DRM). In addition, the consumed energy normalized by time during the DRM reaction in this current-assisted catalysis is sixfold lower (11.0 kJ min -1 ) than that in conventional heating systems (68.4 kJ min -1 ). © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  16. Electronic states of carbon alloy catalysts and nitrogen substituent effects on catalytic activity

    Science.gov (United States)

    Hata, Tomoyuki; Ushiyama, Hiroshi; Yamashita, Koichi

    2013-03-01

    In recent years, Carbon Alloy Catalysts (CACs) are attracting attention as a candidate for non-platinum-based cathode catalysts in fuel cells. Oxygen reduction reactions at the cathode are divided into two elementary processes, electron transfer and oxygen adsorption. The electron transfer reaction is the rate-determining, and by comparison of energy levels, catalytic activity can be evaluated quantitatively. On the other hand, to begin with, adsorption mechanism is obscure. The purpose of this study is to understand the effect of nitrogen substitution and oxygen adsorption mechanism, by first-principle electronic structure calculations for nitrogen substituted models. To reproduce the elementary processes of oxygen adsorption, we assumed that the initial structures are formed based on the Pauling model, a CACs model and nitrogen substituted CACs models in which various points are replaced with nitrogen. When we try to focus only on the DOS peaks of oxygen, in some substituted model that has high adsorption activity, a characteristic partial occupancy state was found. We conclude that this state will affect the adsorption activity, and discuss on why partially occupied states appear with simplification by using an orbital correlation diagram.

  17. Activated carbon as catalyst for microwave-assisted wet peroxide oxidation of aromatic hydrocarbons.

    Science.gov (United States)

    Garcia-Costa, Alicia L; Lopez-Perela, Lucia; Xu, Xiyan; Zazo, Juan A; Rodriguez, Juan J; Casas, Jose A

    2018-05-21

    This paper addresses the removal of four aromatic hydrocarbons typically found in petrochemical wastewater: benzene (B), toluene (T), o-xylene (X), and naphthalene (N), by microwave-assisted catalytic wet peroxide oxidation (MW-CWPO) using activated carbon (AC) as catalyst. Under the studied conditions, complete pollutant elimination (B, 1.28 mM; T, 1.09 mM; X, 0.94 mM; and N, 0.78 mM) was achieved, with more than 90% TOC removal after only 15-min reaction time, working at 120 °C, pH 0  = 3, AC at 1 g L -1 , and H 2 O 2 at the stoichiometric dose. Furthermore, in the case of toluene, naphthalene, and xylene, the hydroxylation and breakdown of the ring is very rapid and toxic intermediates were not detected. The process follows two steps: (i) pollutant adsorption onto AC followed by (ii) adsorbed compounds oxidation. Thus, MW-CWPO with AC as catalyst appears a promising way for a fast and effective process for B, T, X, and N removal in aqueous phase.

  18. 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.

  19. Highly stable and active Ni-doped ordered mesoporous carbon catalyst on the steam reforming of ethanol application

    Directory of Open Access Journals (Sweden)

    Josh Y.Z. Chiou

    2017-02-01

    Full Text Available A novel one-step direct synthesis of nickel embedded in an ordered mesoporous carbon catalyst (NiOMC is done in a basic medium of nonaqueous solution by a solvent evaporation-induced self-assembly process. The NiOMC sample is characterized by a variety of analytical and spectroscopy techniques, e.g., N2 adsorption/desorption isotherm measurement, X-ray diffraction (XRD, transmission electron microscopy (TEM and temperature-programed reduction (TPR. In this study, the NiOMC catalyst is found to exhibit superior catalytic activity for the steam reforming of ethanol (SRE, showing high hydrogen selectivity and durability. Ethanol can be completely converted at 350 °C over the NiOMC catalyst. Also, the durability of the NiOMC catalyst on the SRE reaction exceeds 100 h at 450 °C, with SH2 approaching 65% and SCO of less than 1%.

  20. 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. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

    NARCIS (Netherlands)

    Johansson, A.-C.; Larsen, J.V.; Verheijen, M.A.; Haugshøj, K.B.; Clausen, H.; Kessels, W.M.M.; Christensen, L.H.; Thomsen, E.V.

    2014-01-01

    Pt-Ru catalysts of various compositions, between 0 and 100 at.% 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

  2. Synthesis of a highly active carbon-supported Ir-V/C catalyst for the hydrogen oxidation reaction in PEMFC

    International Nuclear Information System (INIS)

    Li Bing; Qiao Jinli; Yang Daijun; Zheng Junsheng; Ma Jianxin; Zhang Jiujun; Wang Haijiang

    2009-01-01

    The active, carbon-supported Ir and Ir-V nanoclusters with well-controlled particle size, dispersity, and composition uniformity, have been synthesized via an ethylene glycol method using IrCl 3 and NH 4 VO 3 as the Ir and V precursors. The nanostructured catalysts were characterized by X-ray diffraction and high-resolution transmission electron microscopy. The catalytic activities of these carbon-supported nanoclusters were screened by applying on-line cyclic voltammetry and electrochemical impedance spectroscopy techniques, which were used to characterize the electrochemical properties of fuel cells using several anode Ir/C and Ir-V/C catalysts. It was found that Ir/C and Ir-V/C catalysts affect the performance of electrocatalysts significantly based on the discharge characteristics of the fuel cell. The catalyst Ir-V/C at 40 wt.% displayed the highest catalytic activity to hydrogen oxidation reaction and, therefore, high cell performance is achieved which results in a maximum power density of 563 mW cm -2 at 0.512 V and 70 deg. C in a real H 2 /air fuel cell. This performance is 20% higher as compared to the commercial available Pt/C catalyst. Fuel cell life test at a constant current density of 1000 mA cm -2 in a H 2 /O 2 condition shows good stability of anode Ir-V/C after 100 h of continuous operation.

  3. Hydrogen adsorption on activated carbon nanotubes with an atomic-sized vanadium catalyst investigated by electrical resistance measurements

    International Nuclear Information System (INIS)

    Im, Ji Sun; Yun, Jumi; Kang, Seok Chang; Lee, Sung Kyu; Lee, Young-Seak

    2012-01-01

    Activated multi-walled carbon nanotubes were prepared with appended vanadium as a hydrogen storage medium. The pore structure was significantly improved by an activation process that was studied using Raman spectroscopy, field emission transmission electron microscopy and pore analysis techniques. X-ray photoelectron spectroscopy and X-ray diffraction results reveal that the vanadium catalyst was introduced into the carbon nanotubes in controlled proportions, forming V 8 C 7 . The improved pore structure functioned as a path through the carbon nanotubes that encouraged hydrogen molecule adsorption, and the introduced vanadium catalyst led to high levels of hydrogen storage through the dissociation of hydrogen molecules via the spill-over phenomenon. The hydrogen storage behavior was investigated by electrical resistance measurements for the hydrogen adsorbed on a prepared sample. The proposed mechanism of hydrogen storage suggests that the vanadium catalyst increases not only the amount of hydrogen that is stored but also the speed at which it is stored. A hydrogen storage capacity of 2.26 wt.% was achieved with the activation effects and the vanadium catalyst at 30 °C and 10 MPa.

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

    Directory of Open Access Journals (Sweden)

    Viviana Ospina

    2015-05-01

    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.

  5. The Reduction Reaction of Dissolved Oxygen in Water by Hydrazine over Platinum Catalyst Supported on Activated Carbon Fiber

    Energy Technology Data Exchange (ETDEWEB)

    Park, K.K.; Moon, J.S. [Korea Electric Power Research Institute, Taejon (Korea)

    1999-07-01

    The reduction reaction of dissolved oxygen (DO) by hydrazine was investigated on activated carbon fiber (ACF) and Pt/ACF catalysts using a batch reactor with an external circulating loop. The ACF itself showed catalytic activity and this was further improved by supporting platinum on ACF. The catalytic role platinum is ascribed to its acceleration of hydrazine decomposition, based on electric potential and current measurements as well as the kinetic study. (author). 15 refs., 13 figs.

  6. Synthesis of SnO{sub 2}-activated carbon fiber hybrid catalyst for the removal of methyl violet from water

    Energy Technology Data Exchange (ETDEWEB)

    Li, Jia, E-mail: mse_lij@ujn.edu.cn [School of Material Science and Engineering, University of Jinan, Jinan 250022 (China); Ng, Dickon H.L. [Department of Physics, The Chinese University of Hong Kong, Shatin, Hong Kong (China); Song, Peng; Kong, Chao; Song, Yi [School of Material Science and Engineering, University of Jinan, Jinan 250022 (China)

    2015-04-15

    Graphical abstract: - Highlights: • A new biomass route for the synthesis of SnO{sub 2}/ACF hybrid catalyst was proposed. • The original fibrous structure of kapok fiber was retained in the SnO{sub 2}/ACF hybrid catalyst. • SnO{sub 2}/ACF hybrid catalyst exhibited high BET surface area (647–897 m{sup 2}/g) and large pore volume (0.36–0.56 cm{sup 3} g{sup −1}). • High microwave-induced catalytic activity for methyl violet degradation was obtained. - Abstract: SnO{sub 2}/activated carbon fiber (ACF) hybrid catalyst was synthesized from kapok precursor via a two-step process involving pore-fabricating and self-assembly of SnO{sub 2} nanoparticles. The morphology and phase structure of the obtained samples were characterized by X-ray diffraction, field emission scanning electron microscope, high resolution transmission electron microscopy and N{sub 2} adsorption-desorption isotherm. These results demonstrated that the synthesized SnO{sub 2}/ACF retained the hollow-fiber structure of kapok fibers. SnO{sub 2} nanoparticles dispersed uniformly over the ACF support. The obtained hybrid catalyst showed porous structure with high surface area (647–897 m{sup 2}/g) and large pore volume (0.36–0.56 cm{sup 3} g{sup −1}). In addition, the catalytic activities of the obtained samples for methyl violet degradation under microwave irradiation were also evaluated. It was found that the SnO{sub 2}/ACF catalyst exhibited high catalytic activity for methyl violet degradation due to the synergistic effect of microwave and SnO{sub 2}/ACF catalyst.

  7. 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.

  8. Effect of glassy carbon properties on the electrochemical deposition of platinum nano-catalyst and its activity for methanol oxidation

    Directory of Open Access Journals (Sweden)

    SANJA TERZIC

    2007-02-01

    Full Text Available The effects of the properties of glassy carbon on the deposition of platinum particles and the electrocatalytic activity of platinum supported on glassy carbon (GC/Pt for methanol oxidation in alkaline and acidic solutions were studied. Platinum was potentiostatically deposited on two glassy carbon samples, thermally treated at different temperatures, which were either polished or anodicaly polarised in acid (GCOX-AC/Pt and in alkali (GCOX-AL/Pt. Anodic polarisation of glassy carbon, either in alkaline or acidic solution, enhances the activity of both types of GC/Pt electrodes for methanol oxidation. The activity of the catalysts follows the change in the properties of the glassy carbon support upon anodic treatment. The specific activity of the GCOX-AL/Pt electrode for this reaction in alkali is increased only a few times in comparison with the activity of the GC/Pt one. On the other hand, the specific activity of the GCOX-AC/Pt electrode for methanol oxidation in acid is about one order of magnitude higher than that of the GC/Pt electrode. The role of the substrate on the properties of catalyst is discussed in detail.

  9. Systematically controlled pore system of ordered mesoporous carbons using phosphoric acid as the in situ generated catalysts for carbonization and activation

    Energy Technology Data Exchange (ETDEWEB)

    Jin, Xing; Lee, Chang Hyun; Kim, Jin Hoe; You, Dae Jong; Shon, Jeong Kuk; Kim, Ji Man [Dept. of Chemistry, Sungkyunkwan University, Suwon (Korea, Republic of); Pak, Chan Ho [Fuel Cell Group, Corporate R and D Center, Samsung SDI Co. Ltd., Yongin (Korea, Republic of)

    2015-08-15

    We report on a facile synthesis of the ordered mesoporous carbon (OMC) materials with systematically controlled microporosity and mesoporosity simultaneously through the nano-replication route using phosphoric acid as the acid catalyst and activation agent. The use of phosphoric acid affects the pore structures of OMC materials, such as the formation of numerous micropores by activation of the carbon framework and the enlargement of mesopores by spontaneous phase separation during the carbonization. The mesopore sizes, surface areas, total pore volumes, and micropore volumes of the OMC materials are highly dependent on the phosphoric acid content and can be systematically controlled in the range 3.7–7.5 nm, 1027–2782 m{sup 2} g{sup -1}, 1.12–3.53 cm{sup 3} g{sup -1} and 0.34–0.95 cm{sup 3} g{sup -1}, respectively. OMC materials with systematically controlled pore structures were successfully synthesized using phosphoric acid as the carbonization catalyst and mesoporous silica materials with cubic Ia3d and 2-D hexagonal mesostructures as the templates. The phosphoric acid in the synthesis of ordered mesoporous carbon materials acts as the chemical activating agent for micropore generation of the carbon framework and pore-expanding agent for controlling of mesopore size, in addition to functioning as the acid catalyst. The present synthesis pathway is very useful for preparing OMC materials with tunable mesopore sizes and well-developed microporosities at the same time.

  10. Improvement of activated carbons as oxygen reduction catalysts in neutral solutions by ammonia gas treatment and their performance in microbial fuel cells

    KAUST Repository

    Watson, Valerie J.; Nieto Delgado, Cesar; Logan, Bruce E.

    2013-01-01

    Commercially available activated carbon (AC) powders from different precursor materials (peat, coconut shell, coal, and hardwood) were treated with ammonia gas at 700 C to improve their performance as oxygen reduction catalysts in neutral p

  11. The influence of Mn species on the SO{sub 2} removal of Mn-based activated carbon catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Qu, Yi-Fan [College of Architecture and Environment, Sichuan University, Chengdu 610065 (China); Guo, Jia-Xiu, E-mail: guojiaxiu@scu.edu.cn [College of Architecture and Environment, Sichuan University, Chengdu 610065 (China); National Engineering Technology Research Center for Flue Gas Desulfurization, Chengdu 610065 (China); Chu, Ying-Hao [College of Architecture and Environment, Sichuan University, Chengdu 610065 (China); National Engineering Technology Research Center for Flue Gas Desulfurization, Chengdu 610065 (China); Sun, Ming-Chao [College of Architecture and Environment, Sichuan University, Chengdu 610065 (China); Yin, Hua-Qiang, E-mail: hqyin@scu.edu.cn [College of Architecture and Environment, Sichuan University, Chengdu 610065 (China); National Engineering Technology Research Center for Flue Gas Desulfurization, Chengdu 610065 (China)

    2013-10-01

    Using Mn(NO{sub 3}){sub 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 SO{sub 2} were investigated. MnO and Mn{sub 3}O{sub 4} coexist in catalysts calcined at 650 and 800 °C and exhibit best SO{sub 2} removal ability, whereas Mn{sub 2}O{sub 3} formed in the catalyst calcined at 500 °C and shows poor activity. After treatment by nitric acid, the C=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 MnO{sub 2}. And this change directly results in a decrease of activity. But the SO{sub 2} removal rate has been maintained in the range of 30–40%, indicating that MnO{sub 2} still has a certain SO{sub 2} removal ability.

  12. The influence of Mn species on the SO2 removal of Mn-based activated carbon catalysts

    International Nuclear Information System (INIS)

    Qu, Yi-Fan; Guo, Jia-Xiu; Chu, Ying-Hao; Sun, Ming-Chao; Yin, Hua-Qiang

    2013-01-01

    Using Mn(NO 3 ) 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 SO 2 were investigated. MnO and Mn 3 O 4 coexist in catalysts calcined at 650 and 800 °C and exhibit best SO 2 removal ability, whereas Mn 2 O 3 formed in the catalyst calcined at 500 °C and shows poor activity. After treatment by nitric acid, the C=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 MnO 2 . And this change directly results in a decrease of activity. But the SO 2 removal rate has been maintained in the range of 30–40%, indicating that MnO 2 still has a certain SO 2 removal ability.

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

    Science.gov (United States)

    Granite, Evan J [Wexford, PA; Pennline, Henry W [Bethel Park, PA

    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.

  14. Microwave-activated Ni/carbon catalysts for highly selective hydrogenation of nitrobenzene to cyclohexylamine.

    Science.gov (United States)

    Lu, Xinhuan; He, Jie; Jing, Run; Tao, Peipei; Nie, Renfeng; Zhou, Dan; Xia, Qinghua

    2017-06-01

    Biocarbon supported Ni catalysts have been prepared by facile impregnation of Ni species by microwave-heating and used for selective hydrogenation of nitrobenzene to cyclohexylamine. These catalysts were characterized by X-ray diffraction, Raman spectra, N2 sorption measurement, X-ray photoelectron spectroscopy, temperature programmed reduction of H2 and H2 temperature-programmed desorption. The morphology and particle size of catalysts were imaged by scanning electron microscope and transmission electron microscope. For the hydrogenation of nitrobenzene to cyclohexylamine, 10%Ni/CSC-II(b) exhibits the best catalytic activity to achieve 100 mol% conversion of nitrobenzene and 96.7% selectivity of cyclohexylamine under reaction conditions of 2.0 MPa H2 and 200 °C, ascribed to high dispersion of Ni species and formation of nanosized Ni particles on the support aided by microwave-heating. Thus-prepared Ni/CSC catalyst is greatly activated, in which the addition of precious metal like Rh is totally avoided.

  15. Non-carbon titanium cobalt nitride nanotubes supported platinum catalyst with high activity and durability for methanol oxidation reaction

    Science.gov (United States)

    Chen, Xiaoxiang; Li, Wuyi; Pan, Zhanchang; Xu, Yanbin; Liu, Gen; Hu, Guanghui; Wu, Shoukun; Li, Jinghong; Chen, Chun; Lin, Yingsheng

    2018-05-01

    Titanium cobalt nitride nanotubes (Ti0.95Co0.05N NTs) hybrid support, a novel robust non-carbon support material prepared by solvothermal and post-nitriding processes, is further decorated with Pt nanoparticles for the electrooxidation of methanol. The catalyst is characterized by X-ray diffraction (XRD), nitrogen adsorption/desorption, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and electrochemical measurements. The morphology, structure and composition of the synthesized Ti0.95Co0.05N NTs suggest that the nanotube wall is porous and consists of homogeneous cohesively attached nitrides nanocube particles. Notable, Ti0.95Co0.05N NTs supported Pt catalyst exhibits significantly improved catalytic activity and durability for methanol electrooxidation compared with the conventional JM Pt/C catalyst. The experimental data indicate that enhanced catalytic activity and stability of Pt/Ti0.95Co0.05N NTs towards methanol electrooxidation might be mainly attributed to the tubular nanostructures and synergistic effect introduced by the Co doping. Both of them are playing an important role in improving the activity and durability of the Ti0.95Co0.05N NTs catalyst.

  16. 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)

    Dhawane, Sumit H.; Kumar, Tarkeshwar; Halder, Gopinath

    2015-01-01

    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

  17. Modifiers in rhodium catalysts for carbon monoxide hydrogenation: Structure-activity relationships

    Energy Technology Data Exchange (ETDEWEB)

    Bhore, N. A.

    1989-05-01

    This report is aimed at identifying interesting modified rhodium systems and elucidating structure-activity relationships in these systems with the overall goal of understanding the scientific issues in the catalytic conversion of syngas to oxygenates. Specific additives (sodium and molybdenum) are selected based on the scoping experiments. The effect of the additives on supported rhodium catalysts is then investigated. Throughout the investigation, experiments and analysis were performed on real systems instead of ideal systems. 374 refs., 82 figs., 57 tabs.

  18. Effects of γ- and x-irradiation upon activity and selectivity of a supported silver catalyst in the oxidation of ethylene and carbon monoxide

    International Nuclear Information System (INIS)

    Mora Vallejo, R.J.

    1975-01-01

    Effects of γ and x-radiation on catalytic selectivity of supported silver catalysts for production of ethylene oxide via ethylene oxidation were compared by determination of radio-induced changes in conversion-yield profiles. Influence of photon energy on the kinetics of the irradiation process was studied by determination of conversion-yield profiles, using samples of catalyst exposed to x-rays of different mean photon energy and γ-rays for different cumulative periods of time. The effect of γ-radiation on catalytic activity of the same silver catalysts for carbon monoxide oxidation was analyzed by determination of the reaction kinetics before and after catalyst irradiation

  19. Synthesis of Single-Walled Carbon Nanotubes: Effects of Active Metals, Catalyst Supports, and Metal Loading Percentage

    Directory of Open Access Journals (Sweden)

    Wei-Wen Liu

    2013-01-01

    Full Text Available The effects of active metals, catalyst supports, and metal loading percentage on the formation of single-walled carbon nanotubes (SWNTs were studied. In particular, iron, cobalt, and nickel were investigated for SWNTs synthesis. Iron was found to grow better-quality SWNTs compared to cobalt and nickel. To study the effect of catalyst supports, magnesium oxide, silicon oxide, and aluminium oxide were chosen for iron. Among the studied supports, MgO was identified to be a suitable support for iron as it produced SWNTs with better graphitisation determined by Raman analysis. Increasing the iron loading decreased the quality of SWNTs due to extensive agglomeration of the iron particles. Thus, lower metal loading percentage is preferred to grow better-quality SWNTs with uniform diameters.

  20. 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.

  1. 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%. Copyright © 2016 Elsevier B.V. All rights reserved.

  2. Influence of Micropore and Mesoporous in Activated Carbon Air-cathode Catalysts on Oxygen Reduction Reaction in Microbial Fuel Cells

    International Nuclear Information System (INIS)

    Liu, Yi; Li, Kexun; Ge, Baochao; Pu, Liangtao; Liu, Ziqi

    2016-01-01

    In this study, carbon samples with different micropore and mesoporous structures are prepared as air-cathode catalyst layer to explore the role of pore structure on oxygen reduction reaction. The results of linear sweep voltammetry and power density show that the commercially-produced activated carbon (CAC) has the best electrochemical performance, and carbon samples with only micropore or mesoporous show lower performance than CAC. Nitrogen adsorption-desorption isotherms analysis confirm that CAC has highest surface area (1616 m 2 g −1 ) and a certain amount of micropore and mesoporous. According to Tafel plot and rotating disk electrode, CAC behaves the highest kinetic activity and electron transfer number, leading to the improvement of oxygen reduction reaction. The air permeability test proves that mesoporous structure enhance oxygen permeation. Carbon materials are also analyzed by In situ Fourier Transform Infrared Spectroscopy and H 2 temperature programmed reduction, which indicate that micropore provide active sites for catalysis. In a word, micropore and mesoporous together would improve the electrochemical performance of carbon materials.

  3. Chromium oxide over activated carbons as catalyst for oxidative dehydrogenation of isobutane

    International Nuclear Information System (INIS)

    Cardenas, Agobardo; Acero Fabio N; Diaz, Jose de J

    2007-01-01

    The functional groups at the surface of an activated carbon Norit ROX 08 were modified through reaction with nitric acid, 8.8% 0 2 in N 2 and H 2 . the modified carbons were impregnated with a CrO 3 aqueous solution and used in the oxidative dehydrogenation of isobutane to isobutene (ODH). The formation of isobutene was observed at 443 k, with a maximum selectivity of 85% and a yield of 9%

  4. Graphitic carbon nitride induced activity enhancement of OMS-2 catalyst for pollutants degradation with peroxymonosulfate

    Science.gov (United States)

    Li, Jun; Fang, Jia; Gao, Long; Zhang, Jingwen; Ruan, Xinchao; Xu, Aihua; Li, Xiaoxia

    2017-04-01

    Low valent manganese species and surface oxygen vacancies in OMS-2 play an important role in catalytic reactions, and it is highly desirable and challenging to develop a feasible strategy of increasing the Mn(II) and Mn(III) species concentration in the oxide. Herein, the OMS-2/g-C3N4 hybrids (OMS-2/CN) were prepared by a facile refluxing approach. It was found that the MnOx precursor from the reaction of KMnO4 and MnSO4 was transformed into OMS-2 nanofibers with the formation of more Mn(II) and Mn(III) species in OMS-2 and the destruction and oxidation of g-C3N4. The hybrids exhibited higher efficiency for pollutants degradation in the presence of PMS than the pure OMS-2 or g-C3N4. There was a linear correlation between the specific initial rate and the ratio of Mn(II + III)/Mn(IV). Mechanism investigation indicated that high active manganese species or caged radicals were produced through the oxidation of Mn(II) and Mn(III) by PMS and contributed to the degradation reaction. During five consecutive cycles, the catalyst exhibited good reusability and stability. Therefore, the OMS-2/CN hybrids are promising catalysts for wastewater treatment with PMS as the oxidant.

  5. Effect of the relationship between particle size, inter-particle distance, and metal loading of carbon supported fuel cell catalysts on their catalytic activity

    Science.gov (United States)

    Corradini, Patricia Gon; Pires, Felipe I.; Paganin, Valdecir A.; Perez, Joelma; Antolini, Ermete

    2012-09-01

    The effect of the relationship between particle size ( d), inter-particle distance ( x i ), and metal loading ( y) of carbon supported fuel cell Pt or PtRu catalysts on their catalytic activity, based on the optimum d (2.5-3 nm) and x i / d (>5) values, was evaluated. It was found that for y fuel cell electrode than that using catalysts with y ethanol oxidation on PtRu/C catalysts with same particle size and same degree of alloying but different metal loading. Tests in direct ethanol fuel cells showed that, compared to 20 wt% PtRu/C, the negative effect of the lower x i / d on the catalytic activity of 30 and 40 wt% PtRu/C catalysts was superior to the positive effect of the thinner catalyst layer.

  6. 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...

  7. Microstructural Properties and HDS Activity of CoMo Catalysts Supported on Activated Carbon, Al2O3, ZrO2 and TiO2

    Czech Academy of Sciences Publication Activity Database

    Soukup, Karel; Procházka, Martin; Kaluža, Luděk

    2015-01-01

    Roč. 43, č. 2015 (2015), s. 841-846 ISSN 1974-9791. [International Conference on Chemical and Process Engineering - ICheaP12 /12./. Milano, 19.05.2015-22.05.2015] R&D Projects: GA ČR GAP106/11/0902 Institutional support: RVO:67985858 Keywords : CoMo catalysts * surface area * activated carbon Subject RIV: CF - Physical ; Theoretical Chemistry

  8. Simple synthesis of mesoporous FeNi/graphitic carbon nanocomposite catalysts and study on their activities in catalytic cracking of toluene

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Yangang, E-mail: ygwang8136@gmail.com [Department of Environmental Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093 (China); Chen, Yuting; Yao, Mingcui [Department of Environmental Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093 (China); Qin, Hengfei; Kang, Shifei; Li, Xi [Department of Environmental Science and Engineering, Fudan University, Shanghai 200433 (China); Zuo, Yuanhui; Zhang, Xiaodong [Department of Environmental Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093 (China); Cui, Li-Feng, E-mail: lifeng.cui@gmail.com [Department of Environmental Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093 (China)

    2015-11-01

    Mesoporous FeNi alloy/graphitic carbon nanocomposite catalysts with different Fe/Ni molar ratios have been synthesized through a simple solid–liquid grinding/templating method using mesoporous silica SBA-15 as the template. Metal nitrates and natural soybean oil were respectively used as the magnetic particle precursors and carbon source, which can be infiltrated into the silica template after simple impregnation, grinding and subsequent heat treatment. X-ray diffraction, nitrogen adsorption–desorption, transmission electron microscopy and thermogravimetric analysis techniques were used to characterize the samples. It is observed that high contents of FeNi alloy nanoparticles with the sizes of 3–6 nm are well dispersed into the walls of graphitic mesoporous carbon matrix, and the resulting nanocomposites have a uniform mesostructure with a high specific surface area and large pore volume. Because of these properties, the obtained FeNi/graphitic carbon nanocomposites can be used as novel catalysts for the catalytic cracking of toluene and exhibit a higher activity and stability than FeNi/commercial activated carbon (AC) catalyst. After a period of 810 min reaction at 700 °C, the toluene conversion on the FeNi/graphitic carbon nanocomposites can be maintained at a level of more than 75% and this value is 2.5 times as high as that of the FeNi/AC catalyst. - Highlights: • Mesoporous FeNi alloy/graphitic carbon nanocomposites (FeNi/GCN) were synthesized. • High contents of FeNi alloy nanoparticles are well embedded into the graphitic carbon walls. • The obtained FeNi/GCN catalysts have a high surface area and uniform mesostructure. • The FeNi/GCN catalysts exhibited excellent catalytic performance in the cracking of toluene.

  9. 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

    (ethylcyclopentadienyl)ruthenium (Ru(EtCp)2), respectively. O2 was used as the reactant in both processes. The composition of the catalysts was easily tuned by varying the Pt-to-Ru ALD cycle ratio. The catalysts were tested toward the CO oxidation and methanol oxidation reaction (MOR) in a three-electrode electrochemical set...

  10. Cobalt-embedded carbon nanofiber derived from a coordination polymer as a highly efficient heterogeneous catalyst for activating oxone in water.

    Science.gov (United States)

    Lin, Kun-Yi Andrew; Tong, Wai-Chi; Du, Yunchen

    2018-03-01

    Carbon fiber (CF) supported cobalt nanoparticles (NPs) are promising catalysts for activating Oxone because carbon is non-metal and earth-abundant, and CF-based catalysts exhibit a high aspect ratio, which affords more accessible and dense catalytic sites. Nevertheless, most of CF-supported catalysts are fabricated by post-synthetic methods, which involve complicated preparations. More importantly, metallic NPs are attached to the outer surface of CF rather than embedded within CF. However, there is still a great demand for developing Co-bearing carbon fibers for Oxone activation via simple and effective methods. Thus, this study proposes to develop a cobalt NP-embedded carbon nanofiber (CCNF) by a simple hydrothermal reaction of Co and nitrilotriacetic acid (NA), followed by one-step carbonization. Owing to the coordinative structure of CoNA, the derivative CCNF exhibits a fibrous carbon matrix embedded with evenly distributed and densely packed Co 3 O 4 and magnetic Co 0 nanoparticles. The fibrous structure, magnetism and embedded Co NPs enable CCNF to be a promising catalyst for Oxone activation. As degradation of Rhodamine B (RhB) is selected as a model reaction, CCNF not only rapidly activates Oxone to fully degrade RhB but also shows a much higher catalytic activity than the most common Oxone activator, Co 3 O 4 . CCNF also exhibits the lowest activation energy than any reported catalysts for Oxone activation to degrade RhB. In addition, CCNF could be re-used to activate Oxone for RhB degradation. These results indicate that CCNF is a conveniently prepared and highly effective fibrous Co/C hybrid material for activating Oxone to oxidize contaminants in water. Copyright © 2017. Published by Elsevier Ltd.

  11. Carbon a support for sulfide catalysts

    NARCIS (Netherlands)

    Vissers, J.P.R.; Lensing, T.J.; Mercx, F.P.M.; Beer, de V.H.J.; Prins, R.

    1983-01-01

    Two types of carbon materials, carbon black composite and carbon covered alumina, were studied for-their use as support for sulfide catalysts. The following parameters were varied: type of carbon black, carbon coverage of the alumina and carbon pretreatment. Pore size distributions were determined

  12. Using ammonium bicarbonate as pore former in activated carbon catalyst layer to enhance performance of air cathode microbial fuel cell

    Science.gov (United States)

    Li, Da; Qu, Youpeng; Liu, Jia; He, Weihua; Wang, Haiman; Feng, Yujie

    2014-12-01

    The rolling catalyst layers in air cathode microbial fuel cells (MFCs) are prepared by introducing NH4HCO3 as pore former (PF) with four PF/activated carbon mass ratios of 0.1, 0.2, 0.3 and 1.0. The maximum power density of 892 ± 8 mW m-2 is obtained by cathodes with the mass ratio of 0.2, which is 33% higher than that of the control reactor (without PF, 671 ± 22 mW m-2). Pore analysis indicates the porosity increases by 38% and the major pore range concentrates between 0.5 μm-0.8 μm which likely facilitates to enrich the active reaction sites compared to 0.8 μm-3.0 μm in the control and other PF-cathodes. In addition, pore structure endows the cathode improved exchange current density by 2.4 times and decreased charge transfer resistance by 44%, which are the essential reasons to enhance the oxygen reduction. These results show that addition of NH4HCO3 proves an effective way to change the porosity and pore distribution of catalyst layers and then enhance the MFC performance.

  13. Effect of gasoline composition on oxidative desulfurization using a phosphotungstic acid/activated carbon catalyst with hydrogen peroxide

    International Nuclear Information System (INIS)

    Xiao, Jing; Wu, Luoming; Wu, Ying; Liu, Bing; Dai, Lu; Li, Zhong; Xia, Qibin; Xi, Hongxia

    2014-01-01

    Highlights: • Concerned with the question why ODS catalyst is not effective for real gasoline. • Reported the strong inhibiting effect of gasoline composition on ODS for the 1st time. • ODS reactivity is suggested to be determined by partial charge on S atom of thiophene. • Proposed approaches to improve ODS selectivity for real gasoline desulfurization. - Abstract: This work is concerned with the question of why oxidative desulfurization (ODS) catalyst that show good catalytic performance for ODS of model gasoline thiophenic compounds is not effective for real gasoline. For the first time, the effects of gasoline composition on ODS using a phosphotungstic acid/activated carbon (HPW/AC) catalyst with H 2 O 2 were investigated. ODS of thiophene, one of the most difficult thiophenic compounds to be oxidized, was studied in a model fuel system, where a high thiophene conversion rate of 90% could be reached in 2 h at 90 °C. However, when applying the ODS to a real gasoline, the ODS conversion rate decreased to only 32%, suggesting a strong inhibiting effect of gasoline composition on ODS. The ODS studies in different model fuels suggested that the inhibiting effect can be ascribed to the competitive adsorption and oxidation with the presence of the alkenes and alkylated aromatic hydrocarbons in real gasoline. The active pi-electrons in alkenes and alkyl groups in alkylated aromatic hydrocarbons may react with polyoxoperoxo species or peroxo-metallate complexes formed by phosphotungstic acid–H 2 O 2 interaction. Additionally, it was indicated that the ODS selectivity followed the order of benzothiophene > trimethylthiophene > dimethylthiophene ∼ methylthiophene > thiophene, suggesting the partial charge on the electron-rich sulfur atom may play a decisive role for its oxidation reactivity. To mitigate the inhibiting effect of gasoline composition on ODS, we propose (a) implementation of selective separation–oxidation processes; (b) choice of suitable

  14. Utilization of Cacao Pod Husk (Theobroma cacao l.) as Activated Carbon and Catalyst in Biodiesel Production Process from Waste Cooking Oil

    Science.gov (United States)

    Rachmat, Devita; Johar Mawarani, Lizda; Dewi Risanti, Doty

    2018-01-01

    Cocoa pod husk (Theobroma cacao l.) is a waste from cocoa beans processing. In this research we employ cocoa pod husk as activated carbon to decrease the value of FFA (Free Fatty Acid) in waste cooking oil and as K2CO3 catalyst in biodiesel production process from waste cooking oil. Cocoa pod husk was crusched and grounded into powder that passed thorugh 60 mesh-screen. As activated carbon, cocoa pod husk was firstly carbonized at three variant temperatures i.e 250°C, 300°C and 350°C. The activation process was done using HCl 2M as activator. Based on the results of XRD and FTIR, the carbonization at all variant temperatures does not cause a significant changes in terms of crystallite structure and water content. The pore of activated carbon started to form in sample that was carbonized at 350°C resulting in pore diameter of 5.14644 nm. This result was supported by the fact that the ability of this activated carbon in reducing the FFA of waste cooking oil was the most pronounced one, i.e. up to 86.7% of FFA. It was found that the performance of cocoa pod husk’s activated carbon in reducing FFA is more effective than esterification using H2SO4 which can only decrease 80.8%. On the other hand, the utilization as K2CO3 catalyst was carried out by carbonization at temperature 650°C and extraction using aquadest solvent. The extraction of cocoa pod husk produced 7.067% K2CO3 catalyst. According to RD results the fraction of K2CO3 compound from the green catalysts is the same as the commercial (SAP, 99%) that is ≥ 60%. From the obtained results, the best yield percentage was obtained using K2CO3 catalyst from cacao pod husk extract, i.e. 73-85%. To cope with biodiesel conversion efficiency, a two-step process consisting pretreatment with activated carbon carbonized at 350°C and esterification with K2CO3 from cocoa pod husk catalyst was developed. This two-step process could reach a high conversion of 85%. From the results it was clear that the produced

  15. Effect of the relationship between particle size, inter-particle distance, and metal loading of carbon supported fuel cell catalysts on their catalytic activity

    Energy Technology Data Exchange (ETDEWEB)

    Gon Corradini, Patricia; Pires, Felipe I.; Paganin, Valdecir A.; Perez, Joelma, E-mail: jperez@iqsc.usp.br [Instituto de Quimica de Sao Carlos, USP (Brazil); Antolini, Ermete [Scuola di Scienza dei Materiali (Italy)

    2012-09-15

    The effect of the relationship between particle size (d), inter-particle distance (x{sub i}), and metal loading (y) of carbon supported fuel cell Pt or PtRu catalysts on their catalytic activity, based on the optimum d (2.5-3 nm) and x{sub i}/d (>5) values, was evaluated. It was found that for y < 30 wt%, the optimum values of both d and x{sub i}/d can be always obtained. For y {>=} 30 wt%, instead, the positive effect of a thinner catalyst layer of the fuel cell electrode than that using catalysts with y < 30 wt% is concomitant to a decrease of the effective catalyst surface area due to an increase of d and/or a decrease of x{sub i}/d compared to their optimum values, with in turns gives rise to a decrease in the catalytic activity. The effect of the x{sub i}/d ratio has been successfully verified by experimental results on ethanol oxidation on PtRu/C catalysts with same particle size and same degree of alloying but different metal loading. Tests in direct ethanol fuel cells showed that, compared to 20 wt% PtRu/C, the negative effect of the lower x{sub i}/d on the catalytic activity of 30 and 40 wt% PtRu/C catalysts was superior to the positive effect of the thinner catalyst layer.

  16. Catalyst for Carbon Monoxide Oxidation

    Science.gov (United States)

    Davis, Patricia; Brown, Kenneth; VanNorman, John; Brown, David; Upchurch, Billy; Schryer, David; Miller, Irvin

    2010-01-01

    In many applications, it is highly desirable to operate a CO2 laser in a sealed condition, for in an open system the laser requires a continuous flow of laser gas to remove the dissociation products that occur in the discharge zone of the laser, in order to maintain a stable power output. This adds to the operating cost of the laser, and in airborne or space applications, it also adds to the weight penalty of the laser. In a sealed CO2 laser, a small amount of CO2 gas is decomposed in the electrical discharge zone into corresponding quantities of CO and O2. As the laser continues to operate, the concentration of CO2 decreases, while the concentrations of CO and O2 correspondingly increase. The increasing concentration of O2 reduces laser power, because O2 scavenges electrons in the electrical discharge, thereby causing arcing in the electric discharge and a loss of the energetic electrons required to boost CO2 molecules to lasing energy levels. As a result, laser power decreases rapidly. The primary object of this invention is to provide a catalyst that, by composition of matter alone, contains chemisorbed water within and upon its structure. Such bound moisture renders the catalyst highly active and very long-lived, such that only a small quantity of it needs to be used with a CO2 laser under ambient operating conditions. This object is achieved by a catalyst that consists essentially of about 1 to 40 percent by weight of one or more platinum group metals (Pt, Pd, Rh, Ir, Ru, Os, Pt being preferred); about 1 to 90 percent by weight of one or more oxides of reducible metals having multiple valence states (such as Sn, Ti, Mn, Cu, and Ce, with SnO2 being preferred); and about 1 to 90 percent by weight of a compound that can bind water to its structure (such as silica gel, calcium chloride, magnesium sulfate, hydrated alumina, and magnesium perchlorate, with silica gel being preferred). Especially beneficial results are obtained when platinum is present in the

  17. Catalytic oxidation of sulfide in drinking water treatment: activated carbon as catalyst; Katalytische Oxidation von Sulfid bei der Trinkwasseraufbereitung: Aktivkohle als Katalysator

    Energy Technology Data Exchange (ETDEWEB)

    Hultsch, V; Grischek, T; Wolff, D; Worch, E [Technische Univ. Dresden (Germany). Inst. fuer Wasserchemie; Gun, J [Hebrew Univ. of Jerusalem (Israel). Div. of Environmental Sciences, Fredy and Nadine Herrmann School of Applied Science

    2001-07-01

    In regions with warm climate and limited water resources high sulfide concentrations in groundwater can cause problems during drinking water treatment. Aeration of the raw water is not always sufficient to ensure the hydrogen sulfide concentration below the odour threshold value for hydrogen sulfide. As an alternative, activated carbon can be used as a catalyst for sulfide oxidation of raw water. The use of different types of activated carbon was investigated in kinetic experiments. Both Catalytic Carbon from Calgon Carbon and granulated activated carbon from Norit showed high catalytic activities. The results of the experiments are discussed with regard to the practical use of activated carbon for the elimination of hydrogen sulfide during drinking water treatment. (orig.)

  18. Synthesis of carbon nanotubes and nanotube forests on copper catalyst

    International Nuclear Information System (INIS)

    Kruszka, Bartosz; Terzyk, Artur P; Wiśniewski, Marek; Gauden, Piotr A; Szybowicz, Mirosław

    2014-01-01

    The growth of carbon nanotubes on bulk copper is studied. We show for the first time, that super growth chemical vapor deposition method can be successfully applied for preparation of nanotubes on copper catalyst, and the presence of hydrogen is necessary. Next, different methods of copper surface activation are studied, to improve catalyst efficiency. Among them, applied for the first time for copper catalyst in nanotubes synthesis, sulfuric acid activation is the most promising. Among tested samples the surface modified for 10 min is the most active, causing the growth of vertically aligned carbon nanotube forests. Obtained results have potential importance in application of nanotubes and copper in electronic chips and nanodevices. (paper)

  19. Facile solid-state synthesis of highly dispersed Cu nanospheres anchored on coal-based activated carbons as an efficient heterogeneous catalyst for the reduction of 4-nitrophenol

    Science.gov (United States)

    Wang, Shan; Gao, Shasha; Tang, Yakun; Wang, Lei; Jia, Dianzeng; Liu, Lang

    2018-04-01

    Coal-based activated carbons (AC) were acted as the support, Cu/AC catalysts were synthesized by a facile solid-state reaction combined with subsequent heat treatment. In Cu/AC composites, highly dispersed Cu nanospheres were anchored on AC. The catalytic activity for 4-nitrophenol (4-NP) was investigated, the effects of activation temperature and copper loading on the catalytic performance were studied. The catalysts exhibited very high catalytic activity and moderate chemical stability due to the unique characteristics of the particle-assembled nanostructures, the high surface area and the porous structure of coal-based AC and the good dispersion of metal particles. Design and preparation of non-noble metal composite catalysts provide a new direction for improving the added value of coal.

  20. Hydrogenation of carbon monoxide over supported palladium catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Fujimoto, K.; Hashimoto, H.; Kunugi, T.

    1978-03-01

    An alumina-supported 2% palladium catalyst had higher activity for carbon monoxide hydrogenation than a silica-supported 2% palladium catalyst, at 250/sup 0/-400/sup 0/C and 1 atm. The addition of lanthanum oxide or thorium oxide, but not of potassium oxide, to the silica-supported catalyst increased the conversion at 350/sup 0/C from 1.1% to 81.0% with a selectivity of 56.1% for methane, 1.4% for C/sub 2/ compounds, 0.1% for C/sub 3/ compounds, and 42.5% for carbon dioxide. Temperature-programed desorption of carbon monoxide in a hydrogen stream showed that of two desorption peaks observed for carbon monoxide, the one at higher temperature corresponded to the carbon monoxide species which hydrogenates to methane and that the area of this peak increased with increasing thorium content of the catalyst. Graphs, tables, and 12 references.

  1. Effect of the relationship between particle size, inter-particle distance, and metal loading of carbon supported fuel cell catalysts on their catalytic activity

    International Nuclear Information System (INIS)

    Gon Corradini, Patricia; Pires, Felipe I.; Paganin, Valdecir A.; Perez, Joelma; Antolini, Ermete

    2012-01-01

    The effect of the relationship between particle size (d), inter-particle distance (x i ), and metal loading (y) of carbon supported fuel cell Pt or PtRu catalysts on their catalytic activity, based on the optimum d (2.5–3 nm) and x i /d (>5) values, was evaluated. It was found that for y i /d can be always obtained. For y ≥ 30 wt%, instead, the positive effect of a thinner catalyst layer of the fuel cell electrode than that using catalysts with y i /d compared to their optimum values, with in turns gives rise to a decrease in the catalytic activity. The effect of the x i /d ratio has been successfully verified by experimental results on ethanol oxidation on PtRu/C catalysts with same particle size and same degree of alloying but different metal loading. Tests in direct ethanol fuel cells showed that, compared to 20 wt% PtRu/C, the negative effect of the lower x i /d on the catalytic activity of 30 and 40 wt% PtRu/C catalysts was superior to the positive effect of the thinner catalyst layer.

  2. Comparative study of activated carbon, natural zeolite, and green sand supports for CuOX and ZnO sites as ozone decomposition catalyst

    Science.gov (United States)

    Azhariyah, A. S.; Pradyasti, A.; Dianty, A. G.; Bismo, S.

    2018-03-01

    This research was based on ozone decomposition in industrial environment. Ozone is harmful to human. Therefore, catalysts were made as a mask filter to decompose ozone. Comparison studies of catalyst supports were done using Granular Activated Carbon (GAC), Natural Zeolite (NZ), and Green Sand (GS). GAC showed the highest catalytic activity compared to other supports with conversion of 98%. Meanwhile, the conversion using NZ was only 77% and GS had been just 27%. GAC had the highest catalytic activity because it had the largest pore volume, which is 0.478 cm3/g. So GAC was used as catalyst supports. To have a higher conversion in ozone decomposition, GAC was impregnated with metal oxide as the active site of the catalyst. Active site comparison was made using CuOX and ZnO as the active site. Morphology, composition, and crystal phase were analyzed using SEM-EDX, XRF, and XRD methods. Mask filter, which contained catalysts for ozone decomposition, was tested using a fixed bed reactor at room temperature and atmospheric pressure. The result of conversion was analyzed using iodometric method. CuOX/GAC and ZnO/GAC 2%-w showed the highest catalytic activity and conversion reached 100%. From the durability test, CuOX/GAC 2%-w was better than ZnO/GAC 2%-w because the conversion of ozone to oxygen reached 100% with the lowest conversion was 70% for over eight hours.

  3. Use of Pyrolyzed Iron Ethylenediaminetetraacetic Acid Modified Activated Carbon as Air–Cathode Catalyst in Microbial Fuel Cells

    KAUST Repository

    Xia, Xue

    2013-08-28

    Activated carbon (AC) is a cost-effective catalyst for the oxygen reduction reaction (ORR) in air-cathode microbial fuel cells (MFCs). To enhance the catalytic activity of AC cathodes, AC powders were pyrolyzed with iron ethylenediaminetetraacetic acid (FeEDTA) at a weight ratio of FeEDTA:AC = 0.2:1. MFCs with FeEDTA modified AC cathodes and a stainless steel mesh current collector produced a maximum power density of 1580 ± 80 mW/m2, which was 10% higher than that of plain AC cathodes (1440 ± 60 mW/m 2) and comparable to Pt cathodes (1550 ± 10 mW/m2). Further increases in the ratio of FeEDTA:AC resulted in a decrease in performance. The durability of AC-based cathodes was much better than Pt-catalyzed cathodes. After 4.5 months of operation, the maximum power density of Pt cathode MFCs was 50% lower than MFCs with the AC cathodes. Pyridinic nitrogen, quaternary nitrogen and iron species likely contributed to the increased activity of FeEDTA modified AC. These results show that pyrolyzing AC with FeEDTA is a cost-effective and durable way to increase the catalytic activity of AC. © 2013 American Chemical Society.

  4. Heterogeneous catalytic ozonation of biologically pretreated Lurgi coal gasification wastewater using sewage sludge based activated carbon supported manganese and ferric oxides as catalysts.

    Science.gov (United States)

    Zhuang, Haifeng; Han, Hongjun; Hou, Baolin; Jia, Shengyong; Zhao, Qian

    2014-08-01

    Sewage sludge of biological wastewater treatment plant was converted into sewage sludge based activated carbon (SBAC) with ZnCl₂ as activation agent, which supported manganese and ferric oxides as catalysts (including SBAC) to improve the performance of ozonation of real biologically pretreated Lurgi coal gasification wastewater. The results indicated catalytic ozonation with the prepared catalysts significantly enhanced performance of pollutants removal and the treated wastewater was more biodegradable and less toxic than that in ozonation alone. On the basis of positive effect of higher pH and significant inhibition of radical scavengers in catalytic ozonation, it was deduced that the enhancement of catalytic activity was responsible for generating hydroxyl radicals and the possible reaction pathway was proposed. Moreover, the prepared catalysts showed superior stability and most of toxic and refractory compounds were eliminated at successive catalytic ozonation runs. Thus, the process with economical, efficient and sustainable advantages was beneficial to engineering application. Copyright © 2014 Elsevier Ltd. All rights reserved.

  5. High-Activity Dealloyed Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Kongkanand, Anusorn [General Motors LLC, Pontiac, MI (United States)

    2014-09-30

    Reduction of costly Pt usage in proton exchange membrane fuel cell electrodes is one of the major challenges towards development and commercialization of fuel cell vehicles. Although few have met the initial-kinetic activity requirements in a realistic fuel cell device, no catalyst material has ever met the demanding fuel cell durability targets set by DOE. In this project, a team of 4 universities and 2 companies came together to investigate a concept that appeared promising in preliminary non-fuel cell tests then to further develop the catalyst to a mature level ready for vehicle implementation. The team consists of academia with technical leadership in their respective areas, a catalyst supplier, and a fuel cell system integrator.The tightly collaborative project enabled development of a highly active and durable catalyst with performance that significantly exceeds that of previous catalysts and meets the DOE targets for the first time (Figure 1A). The catalyst was then further evaluated in full-active-area stack in a realistic vehicle operating condition (Figure 1B). This is the first public demonstration that one can realize the performance benefit and Pt cost reduction over a conventional pure Pt catalyst in a long-term realistic PEMFC system. Furthermore, systematic analyses of a range of catalysts with different performance after fuel cell testing allowed for correlation between catalyst microstructure and its electrocatalytic activity and durability. This will in turn aid future catalyst development.

  6. Activating catalysts with mechanical force

    NARCIS (Netherlands)

    Piermattei, A.; Karthikeyan, S.; Sijbesma, R.P.

    2009-01-01

    Homogeneously catalysed reactions can be ‘switched on’ by activating latent catalysts. Usually, activation is brought about by heat or an external chemical agent. However, activation of homogeneous catalysts with a mechanical trigger has not been demonstrated. Here, we introduce a general method to

  7. Nitrogen-doped carbon nanotubes as a metal catalyst support

    CSIR Research Space (South Africa)

    Mabena, LF

    2011-05-01

    Full Text Available ., which are among the most commonly used heterogeneous catalyst supports (Mart??nez-Me?ndez et al. 2006). Catalyst activity depends on the particle size and appropriate dis- tance between each particle. These catalysts deposited on a support... supported Pt electrodes. Appl Catal B Environ 80:286?295 Maldonado S, Morin S, Stevenson KJ (2006) Structure, composition, and chemical reactivity of carbon nanotubes by selective nitrogen doping. Carbon 44:1429?1437 Mart??nez-Me?ndez S, Henr??quez Y...

  8. Carbonylation of aryl bromides with palladium polyphthalocyanine/active carbon catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Ohkatsu, Y.; Nakazawa, K.; Osa, T.

    1979-11-01

    The reaction of bromobenzene with carbon monoxide over carbon-supported 1.7Vertical Bar3< palladium polyphthalocyanine yielded carbonylated products in the presence of water or methanol and only benzene and dibromobenzene in their absence. At 300/sup 0/C and 1 sec contact time, e.g., the reaction of a 1:2.6:1 mole ratio feed of bromobenzene/methanol/carbon monoxide yielded benzoic acid with 61.7Vertical Bar3< selectivity at 83.2Vertical Bar3< conversion, a 1:0.8:3 feed gave benzoic acid with 84.4Vertical Bar3< selectivity at 40.7Vertical Bar3< conversion. The addition of water instead of methanol gave higher conversions, e.g., a feed of 1:3:1 bromobenzene/water/carbon monoxide yielded benzoic acid with 69.2Vertical Bar3< selectivity at 90.9Vertical Bar3< conversion. Analyses of product distributions obtained in these and autoclaved experiments at 10-50 kg/sq cm carbon monoxide pressure suggested a free radical mechanism.

  9. Nanosized ruthenium particles decorated carbon nanofibers as active catalysts for the oxidation of p-cymene by molecular oxygen

    CSIR Research Space (South Africa)

    Makgwane, PR

    2013-07-01

    Full Text Available demonstrated that the direct participation of the catalyst in p-cymene C-H bond activation occurred via catalytic decomposition of tertiary-butyl hydroperoxide (TBHP), which was added as an initiator, into a free-radical chain initiator rather than the direct H...

  10. Degradation of metaldehyde in water by nanoparticle catalysts and powdered activated carbon.

    Science.gov (United States)

    Li, Zhuojun; Kim, Jong Kyu; Chaudhari, Vrushali; Mayadevi, Suseeladevi; Campos, Luiza C

    2017-07-01

    Metaldehyde, an organic pesticide widely used in the UK, has been detected in drinking water in the UK with a low concentration (doped titanium dioxide nanocatalyst with different concentrations of carbon (C-1.5, C-40, and C-80) for metaldehyde removal from aqueous solutions by adsorption and oxidation via photocatalysis. PAC was found to be the most effective material which showed almost over 90% removal. Adsorption data were well fitted to the Langmuir isotherm model, giving a q m (maximum/saturation adsorption capacity) value of 32.258 mg g -1 and a K L (Langmuir constant) value of 2.013 L mg -1 . In terms of kinetic study, adsorption of metaldehyde by PAC fitted well with a pseudo-second-order equation, giving the adsorption rate constant k 2 value of 0.023 g mg -1  min -1 , implying rapid adsorption. The nanocatalysts were much less effective in oxidising metaldehyde than PAC with the same metaldehyde concentration and 0.2 g L -1 loading concentration of materials under UV light; the maximum removal achieved by carbon-doped titanium dioxide (C-1.5) nanocatalyst was around 15% for a 7.5 ppm metaldehyde solution. Graphical abstract ᅟ.

  11. Electroreduction of oxygen on carbon-supported gold catalysts

    International Nuclear Information System (INIS)

    Erikson, Heiki; Juermann, Gea; Sarapuu, Ave; Potter, Robert J.; Tammeveski, Kaido

    2009-01-01

    The electrochemical reduction of oxygen was studied on Au/C catalysts (20 and 30 wt%) in 0.5 M H 2 SO 4 and 0.1 M KOH solutions using the rotating disk electrode (RDE) method. The thickness of the Au/C-Nafion layers was varied between 1.5 and 10 μm. The specific activity of Au was independent of catalyst loading in both solutions, indicating that the transport of reactants through the catalyst layer does not limit the process of oxygen reduction under these conditions. The mass activity of 20 wt% Au/C catalysts was higher due to smaller particle size. The number of electrons involved in the reaction and the Tafel slopes were found; the values of these parameters are similar to that of bulk polycrystalline gold and indicate that the mechanism of O 2 reduction is not affected by carbon support or the catalyst configuration.

  12. Nitrogen controlled iron catalyst phase during carbon nanotube growth

    Energy Technology Data Exchange (ETDEWEB)

    Bayer, Bernhard C., E-mail: bernhard.bayer@univie.ac.at [Department of Engineering, University of Cambridge, Cambridge CB3 0FA (United Kingdom); Faculty of Physics, University of Vienna, A-1090 Vienna (Austria); Baehtz, Carsten [Institute of Ion Beam Physics and Materials Research, Helmholtz-Zentrum Dresden-Rossendorf, D-01314 Dresden (Germany); Kidambi, Piran R.; Weatherup, Robert S.; Caneva, Sabina; Cabrero-Vilatela, Andrea; Hofmann, Stephan [Department of Engineering, University of Cambridge, Cambridge CB3 0FA (United Kingdom); Mangler, Clemens; Kotakoski, Jani; Meyer, Jannik C. [Faculty of Physics, University of Vienna, A-1090 Vienna (Austria); Goddard, Caroline J. L. [Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS (United Kingdom)

    2014-10-06

    Close control over the active catalyst phase and hence carbon nanotube structure remains challenging in catalytic chemical vapor deposition since multiple competing active catalyst phases typically co-exist under realistic synthesis conditions. Here, using in-situ X-ray diffractometry, we show that the phase of supported iron catalyst particles can be reliably controlled via the addition of NH{sub 3} during nanotube synthesis. Unlike polydisperse catalyst phase mixtures during H{sub 2} diluted nanotube growth, nitrogen addition controllably leads to phase-pure γ-Fe during pre-treatment and to phase-pure Fe{sub 3}C during growth. We rationalize these findings in the context of ternary Fe-C-N phase diagram calculations and, thus, highlight the use of pre-treatment- and add-gases as a key parameter towards controlled carbon nanotube growth.

  13. Activated carbon from orange peels as supercapacitor electrode and catalyst support for oxygen reduction reaction in proton exchange membrane fuel cell

    Directory of Open Access Journals (Sweden)

    M. Dhelipan

    2017-05-01

    Full Text Available Activated carbon is synthesized using orange peel as precursor through chemical activation using H3PO4 and its ability as electrocatalyst support for ORR reaction is examined. The prepared material was subjected to various structural, compositional, morphological and electrochemical studies. For ORR activity, the platinum loaded on activated carbon (Pt/OP-AC was investigated by cyclic voltammograms (CVs recorded in N2 and O2 saturated 0.1 M aqueous HClO4. For supercapacitor performance, three electrode systems was tested in aqueous H2SO4 for feasibility determination and showed electrochemical double layer capacitance (EDLC behaviour which is expected for activated carbon like materials. Electrochemical surface area (ECSA of the activated carbon from orange peel is measured using CV. The physical properties of the prepared carbon are studied using SEM (scanning electron microscope, XRD (X-ray diffraction, Fourier transform infrared (FT-IR spectroscopy and Raman spectroscopy. The AC derived from orange peels delivered a high specific capacitance of 275 F g−1 at 10 mV s-1 scan rate. Hence, this study suggested that orange peels may be considered not only as a potential alternative source for synthesizing carbon supported catalyst for fuel cell application but also highlight the production of low-cost carbon for further applications like supercapacitors.

  14. Influences of species of metals and supports on the hydrogenation activity of carbon-supported metal sulfides catalysts; Tanso biryushi tanji shokubai no suisoka kassei ni taisuru kassei kinzoku oyobi tantaishu no eikyo

    Energy Technology Data Exchange (ETDEWEB)

    Sakanishi, K.; Hasuo, H.; Taniguchi, H.; Nagamatsu, T.; Mochida, I. [Kyushu University, Fukuoka (Japan). Institute of Advanced Material Study

    1996-10-28

    In order to design catalysts suitable for primary liquefaction stage and secondary upgrading stage respectively in the multi-stage liquefaction process, various carbon-supported catalysts were prepared. Catalytic activities of them were investigated for the hydrogenation of 1-methylnaphthalene, to discuss the influences of metals and carbon species on the catalytic activity. Various water soluble and oil soluble Mo and Ni salts were used for NiMo supported catalysts. Among various carbon supports, Ketjen Black (KB) was effective for preparing the catalyst showing the most excellent hydrogenation activity. The KB and Black Pearl 2000 (BP2000) showing high hydrogenation activity were fine particles having high specific surface area more than 1000 m{sup 2}/g and primary particle diameter around 30 nm. This was inferred to contribute to the high dispersion support of active metals. Since such fine particles of carbon exhibited hydrophobic surface, they were suitable for preparing catalysts from the methanol-soluble metals. Although Ni and Mo added iron-based catalysts provided lower aromatic hydrogenation activity, they exhibited liquefaction activity competing with the NiMo/KB catalyst. 3 refs., 1 fig., 3 tabs.

  15. Influence of surface oxygenated groups on the formation of active Cu species and the catalytic activity of Cu/AC catalyst for the synthesis of dimethyl carbonate

    Science.gov (United States)

    Zhang, Guoqiang; Li, Zhong; Zheng, Huayan; Hao, Zhiqiang; Wang, Xia; Wang, Jiajun

    2016-12-01

    Activated carbon (AC) supported Cu catalysts are employed to study the influence of surface oxygenated groups on the formation of active Cu species and the catalytic activity of Cu/AC catalyst for oxidative carbonylation of methanol to dimethyl carbonate (DMC). The AC supports are thermal treated under different temperatures in order to adjust the levels of surface oxygenated groups. The AC supports are characterized by BET, TPD-MS and XRD, and the Cu/AC catalysts are characterized by BET, XRD, TEM, XPS, AAS, CH3OH-TPD and N2O chemisorption. The results show that as the treatment temperature is below 800 °C, the BET surface area of the corresponding AC supports are nearly unchanged and close to that of the original AC (1529.6 m2/g). But as the thermal treatment temperature is elevated from 1000 to 1600 °C, the BET surface area of AC supports gradually decreases from 1407.6 to 972.2 m2/g. After loading of Cu, the BET surface area of copper catalysts is in the range of 834.4 to 1545.3 m2/g, which is slightly less than that of the respective supports. When AC is thermal treated at 400 and 600 °C, the unstable carboxylic acid and anhydrides groups are selectively removed, which has weakened the mobility and agglomeration of Cu species during the calcination process, and thus improve the Cu species dispersion over AC support. But as the treatment temperature is elevated from 600 °C to 1200 °C, the Cu species dispersion begins to decline suggesting further removal of stable surface oxygenated groups is unfavorable for Cu species dispersion. Moreover, higher thermal treatment temperature (above 1200 °C) promotes the graphitization degree of AC and leds to the decrease of Cu loading on AC support. Meanwhile, the removal of surface oxygenated groups by thermal treatment is conducive to the formation of more π-sites, and thus promote the reduction of Cu2+ to Cu+ and Cu0 as active centers. The specific surface area of (Cu+ + Cu0) is improved by thermal treatment of AC

  16. Interfacial charge distributions in carbon-supported palladium catalysts

    DEFF Research Database (Denmark)

    Rao, Radhika G.; Blume, Raoul; Hansen, Thomas Willum

    2017-01-01

    Controlling the charge transfer between a semiconducting catalyst carrier and the supported transition metal active phase represents an elite strategy for fine turning the electronic structure of the catalytic centers, hence their activity and selectivity. These phenomena have been theoretically...... and experimentally elucidated for oxide supports but remain poorly understood for carbons due to their complex nanoscale structure. Here, we combine advanced spectroscopy and microscopy on model Pd/C samples to decouple the electronic and surface chemistry effects on catalytic performance. Our investigations reveal...... treatments can be used to tune the interfacial charge distribution, hereby providing a strategy to rationally design carbon-supported catalysts.Control over charge transfer in carbon-supported metal nanoparticles is essential for designing new catalysts. Here, the authors show that thermal treatments...

  17. In-situ Electrodeposition of Highly Active Silver Catalyst on Carbon Fiber Papers as Binder Free Cathodes for Aluminum-air Battery

    OpenAIRE

    Hong, Qingshui; Lu, Huimin

    2017-01-01

    Carbon fiber papers supported Ag catalysts (Ag/CFP) with different coverage of electro-active site are prepared by electrochemical deposition and used as binder free cathodes in primary aluminum-air (Al-air) battery. Scanning Electron Microscopy and X-ray Diffraction studies are carried out to characterize the as-prepared Ag/CFP air cathodes. Oxygen reduction reaction (ORR) activities on these air cathodes in alkaline solutions are systematic studied. A newly designed aluminum-air cell is use...

  18. Robust non-carbon titanium nitride nanotubes supported Pt catalyst with enhanced catalytic activity and durability for methanol oxidation reaction

    International Nuclear Information System (INIS)

    Xiao, Yonghao; Zhan, Guohe; Fu, Zhenggao; Pan, Zhanchang; Xiao, Chumin; Wu, Shoukun; Chen, Chun; Hu, Guanghui; Wei, Zhigang

    2014-01-01

    By the combination of solvothermal alcoholysis and post-nitriding method, titanium nitride nanotubes (TiN NTs), with high surface area, hollow and interior porous structure are prepared successfully and used at a support for Pt nanoparticles. The TiN NTs supported Pt (Pt/TiN NTs) catalyst displays enhanced activity and durability towards methanol oxidation reaction (MOR) compared with the commercial Pt/C (E-TEK) catalyst. X ray diffraction (XRD), nitrogen adsorption/desorption, transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) measurements are performed to investigate the physicochemical properties of the synthesized catalyst. SEM and TEM images reveal that the wall of the TiN NTs is porous and Pt nanoparticles supported on the dendritic TiN nanocrystals exhibit small size and good dispersion. Effects of inherent corrosion-resistant, tubular and porous nanostructures and electron transfer due to the strong metal–support interactions of TiN NTs contribute to the enhanced catalytic activity and stability of Pt/TiN NTs towards the MOR

  19. Phosphorus poisoning of molybdenum sulfide hydrodesulfurization catalysts supported on carbon and alumina

    NARCIS (Netherlands)

    Bouwens, S.M.A.M.; Vissers, J.P.R.; Beer, de V.H.J.; Prins, R.

    1988-01-01

    Phosphorus-containing Mo sulfide catalysts supported on ¿-Al2O3 and activated carbon were evaluated for their thiophene HDS activities. Phosphorus was added as phosphoric acid to the carrier material prior to the molybdenum component. The thiophene HDS activity of the carbon-supported catalysts was

  20. 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  |  

  1. A novel structure of scalable air-cathode without Nafion and Pt by rolling activated carbon and PTFE as catalyst layer in microbial fuel cells.

    Science.gov (United States)

    Dong, Heng; Yu, Hongbing; Wang, Xin; Zhou, Qixing; Feng, Junli

    2012-11-01

    Single chambered air-cathode microbial fuel cells (MFCs) are promising to be scaled up as sustainable wastewater treatment systems. However, the current air-cathode made by brushing noble metal catalyst and Nafion binder onto carbon matrix becomes one of the biggest bottlenecks for the further development of MFCs due to its high cost, huge labor-consuming and less accuracy. A novel structure of air-cathode was constructed here by rolling activated carbon (AC) and polytetrafluoroethylene (PTFE) as catalyst layer to enhance the reproducibility and improve the performance by an optimized three-phase interface (TPI). Air-cathodes with AC/PTFE ratios of 3, 5, 6, 8 and 11 in the catalyst layer were prepared, and the physical and electrochemical techniques were employed to investigate their surface microstructure and electrochemical characteristics. Uniform cross-linked ropiness networks were observed from the catalyst layer of all the cathodes and increased as the AC/PTFE ratio decreased, while the exchange currents were positively related to this ratio. Maximum power densities (MPDs) decreased as follows: AC/PTFE = 6 (802 mW m(-2) at 3.4 A m(-2)), 5 (704 mW m(-2) at 2.2 mA m(-2)), 8 (647 mW m(-2) at 2.2 A m(-2)), 3 (597 mW m(-2) at 2.1 A m(-2)) and 11 (584 mW m(-2) at 2.0 mA m(-2)), which was due to the changes of both the capacitance characteristics and conductivities according to the electrochemical impedance spectrum (EIS) analysis. This study demonstrated that inexpensive, highly reproducible, high performance and scalable air-cathode can be produced by rolling method without using noble metal and expensive binder. Copyright © 2012 Elsevier Ltd. All rights reserved.

  2. Destruction of Toluene by the Combination of High Frequency Discharge Electrodeless Lamp and Manganese Oxide-Impregnated Granular Activated Carbon Catalyst

    Directory of Open Access Journals (Sweden)

    Jianhui Xu

    2014-01-01

    Full Text Available The destruction of low concentration of toluene (0–30 ppm has been studied under the UV/photogenerated O3/MnO2-impregnated granular activated carbon (MnO2-impregnated GAC process by the combination of self-made high frequency discharge electrodeless lamp (HFDEL with MnO2-impregnated GAC catalyst. Experimental results showed that the initial toluene concentration can strongly affect the concentration of photogenerated O3 from HFDEL and the efficiency and mass rate of destruction of toluene via HFDEL/MnO2-impregnated GAC system. Active oxygen and hydroxyl radicals generated from HFDEL/MnO2-impregnated GAC system played a key role in the decomposition of toluene process and the intermediates formed by photolysis are more prone to be mineralized by the subsequent MnO2-impregnated GAC catalyst compared to the original toluene, resulting in synergistic mineralization of toluene by HFDEL/MnO2-impregnated GAC system. The role of MnO2-impregnated GAC catalyst is not only to eliminate the residual O3 completely but also to enhance the decomposition and mineralization of toluene.

  3. Carbon formation on nickel and nickel-copper alloy catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Alstrup, I.; Soerensen, O.; Rostrup-Nielsen, J.R. [Haldor Topsoe Research Labs., Lyngby (Denmark); Tavares, M.T.; Bernardo, C.A.

    1998-05-01

    Equilibrium, kinetic and morphological studies of carbon formation in CH{sub 4} + H{sub 2}, CO, and CO + H{sub 2} gases on silica supported nickel and nickel-copper catalysts are reviewed. The equilibrium deviates in all cases from graphite equilibrium and more so in CO + CO{sub 2} than in CH{sub 4} + H{sub 2}. A kinetic model based on information from surface science results with chemisorption of CH{sub 4} and possibly also the first dehydrogenation step as rate controlling describes carbon formation on nickel catalyst in CH{sub 4} + H{sub 2} well. The kinetics of carbon formation in CO and CO + H{sub 2} gases are in agreement with CO disproportionation as rate determining step. The presence of hydrogen influences strongly the chemisorption of CO. Carbon filaments are formed when hydrogen is present in the gas while encapsulating carbon dominates in pure CO. Small amounts of Cu alloying promotes while larger amounts (Cu : Ni {>=} 0.1) inhibits carbon formation and changes the morphology of the filaments (``octopus`` carbon formation). Adsorption induced nickel segregation changes the kinetics of the alloy catalysts at high carbon activities. Modifications suggested in some very recent papers on the basis of new results are also briefly discussed. (orig.) 31 refs.

  4. N/S/B-doped graphitized carbon encased Fe species as a highly active and durable catalyst towards oxygen reduction reaction.

    Science.gov (United States)

    Li, Guang-Lan; Cheng, Guang-Chun; Chen, Wen-Wen; Liu, Cai-Di; Yuan, Li-Fang; Yang, Bei-Bei; Hao, Ce

    2018-03-15

    Exploring cost-effective, high-performance and durable non-precious metal catalysts is of great significance for the acceleration of sluggish oxygen reduction reaction (ORR). Here, we report an intriguing heteroatom-doped graphitized carbon encased Fe species composite by introducing N, S and B sequentially. The experimental approach was designed ingeniously for that the FeCl 3 ·6H 2 O could catalyze thiourea to synthesize N, S co-doped carbon materials which would further react with H 3 BO 3 and NH 3 (emerged at the heat-treatment process) to prepare N, S and B co-doped carbon materials (Fe-N/S/B-C). The Fe-N/S/B-C exhibits an impressive ORR activity for its half-wave potential of -0.1 V, which is 36 mV or 19 mV higher than that of the corresponding single or dual doped counterparts (Fe-N-C or Fe-N/S-C) and 31 mV positive than that of Pt/C catalyst, respectively. Further chronoamperometric measurement and accelerated aging test confirm the excellent electrochemical durability of Fe-N/S/B-C with the stable core-shell structure. The remarkable ORR performance and facile preparation method enable Fe-N/S/B-C as a potential candidate in electrochemical energy devices. Copyright © 2017 Elsevier Inc. All rights reserved.

  5. From ionic liquid-modified cellulose nanowhiskers to highly active metal-free nanostructured carbon catalysts for the hydrazine oxidation reaction

    Czech Academy of Sciences Publication Activity Database

    Fragal, E.H.; Fragal, V.H.; Huang, X.; Martins, A.C.; Cellet, T.S.P.; Pereira, G.M.; Mikmeková, Eliška; Rubira, A.F.; Silva, R.; Asefa, T.

    2017-01-01

    Roč. 5, č. 3 (2017), s. 1066-1077 ISSN 2050-7488 Institutional support: RVO:68081731 Keywords : carbonization * catalysts Subject RIV: JA - Electronics ; Optoelectronics, Electrical Engineering OBOR OECD: Physical chemistry Impact factor: 8.867, year: 2016

  6. 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.

  7. TiO2-Containing Carbon Derived from a Metal-Organic Framework Composite: A Highly Active Catalyst for Oxidative Desulfurization.

    Science.gov (United States)

    Bhadra, Biswa Nath; Song, Ji Yoon; Khan, Nazmul Abedin; Jhung, Sung Hwa

    2017-09-13

    A new metal-organic framework (MOF) composite consisting of Ti- and Zn-based MOFs (ZIF-8(x)@H 2 N-MIL-125; in brief, ZIF(x)@MOF) was designed and synthesized. The pristine MOF [H 2 N-MIL-125 (MOF)]- and an MOF-composite [ZIF(30)@MOF]-derived mesoporous carbons consisting of TiO 2 nanoparticles were prepared by pyrolysis (named MDC-P and MDC-C, respectively). MDC-C showed a higher surface area, larger pore sizes, and larger mesopore volumes than MDC-P. In addition, the TiO 2 nanoparticles on MDC-C have more uniform shapes and sizes and are smaller than those of MDC-P. The obtained MDC-C and MDC-P [together with MOF, ZIF(30)@MOF, pure/nanocrystalline TiO 2 , and activated carbon] were applied in the oxidative desulfurization reaction of dibenzothiophene in a model fuel. The MDC-C, even with a lower TiO 2 content than that of MDC-P, showed an outstanding catalytic performance, especially with a very low catalyst dose (i.e., a very high quantity of dibenzothiophene was converted per unit weight of the catalyst), fast kinetics (∼3 times faster than that for MDC-P), and a low activation energy (lower than that for any reported catalyst) for the oxidation of dibenzothiophene. The large mesopores of MDC-C and the well-dispersed/small TiO 2 might be the dominant factors for the superior catalytic conversions. The oxidative desulfurization of other sulfur-containing organic compounds with various electron densities was also studied with MDC-C to understand the mechanism of catalysis. Moreover, the MDC-C catalyst can be reused many times in the oxidative desulfurization reaction after a simple washing with acetone. Finally, composing MOFs and subsequent pyrolysis is suggested as an effective way to prepare a catalyst with well-dispersed active sites, large pores, and high mesoporosity.

  8. Carbon nanotube forests growth using catalysts from atomic layer deposition

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Bingan; Zhang, Can; Esconjauregui, Santiago; Xie, Rongsi; Zhong, Guofang; Robertson, John [Department of Engineering, University of Cambridge, Cambridge CB3 0FA (United Kingdom); Bhardwaj, Sunil [Istituto Officina dei Materiali-CNR Laboratorio TASC, s.s. 14, km 163.4, I-34012 Trieste (Italy); Sincrotone Trieste S.C.p.A., s.s. 14, km 163.4, I-34149 Trieste (Italy); Cepek, Cinzia [Istituto Officina dei Materiali-CNR Laboratorio TASC, s.s. 14, km 163.4, I-34012 Trieste (Italy)

    2014-04-14

    We have grown carbon nanotubes using Fe and Ni catalyst films deposited by atomic layer deposition. Both metals lead to catalytically active nanoparticles for growing vertically aligned nanotube forests or carbon fibres, depending on the growth conditions and whether the substrate is alumina or silica. The resulting nanotubes have narrow diameter and wall number distributions that are as narrow as those grown from sputtered catalysts. The state of the catalyst is studied by in-situ and ex-situ X-ray photoemission spectroscopy. We demonstrate multi-directional nanotube growth on a porous alumina foam coated with Fe prepared by atomic layer deposition. This deposition technique can be useful for nanotube applications in microelectronics, filter technology, and energy storage.

  9. Catalytic activity in reactions of isotopic exchange of carbon monoxide and adsorption properties of catalysts on zinc oxide base

    International Nuclear Information System (INIS)

    Mikheeva, T.M.; Kasatkina, L.A.; Volynkina, A.Ya.

    1987-01-01

    Activity of different zinc oxide samples in reaction of CO homomolecular isotopic exchnge (HMIE) ( 13 C 18 O+ 12 C 16 O= 13 C 16 O+ 12 C 18 O), CO adsorption on ZnO and isotopic exchange between adsorbed and gaseous CO are investigated. The most active is ZnO sample prepared from ZnCO 3 . Quantitative ratio between different with respect to surface strength molecules of adsorbed CO are experimentally determined. It is shown that by increase of ZnO time contact with CO the quantity of adsorbed CO(N σ/0 ), capable of fast exchange with a gaseous phase, is reduced and the quantity of slowly exchanged adsorbed CO is increased. Correlation between decrease of N σ/0 and decrease of CO HMIE with the catalyst holding time in CO medium is stated

  10. In-situ Electrodeposition of Highly Active Silver Catalyst on Carbon Fiber Papers as Binder Free Cathodes for Aluminum-air Battery.

    Science.gov (United States)

    Hong, Qingshui; Lu, Huimin

    2017-06-13

    Carbon fiber papers supported Ag catalysts (Ag/CFP) with different coverage of electro-active site are prepared by electrochemical deposition and used as binder free cathodes in primary aluminum-air (Al-air) battery. Scanning Electron Microscopy and X-ray Diffraction studies are carried out to characterize the as-prepared Ag/CFP air cathodes. Oxygen reduction reaction (ORR) activities on these air cathodes in alkaline solutions are systematic studied. A newly designed aluminum-air cell is used to further determine the cathodes performance under real operation condition and during the test, the Ag/CFP electrodes show outstanding catalytic activity for ORR in concentrated alkaline electrolyte, and no obvious activity degradation is observed after long-time discharge. The electrochemical test results display the dependence of coverage of the electro-active Ag on the catalytic performance of the air cathodes. The resulting primary Al-air battery made from the best-performing cathode shows an impressive discharge peak power density, outperforming that of using commercial nano-manganese catalyst air electrodes.

  11. Tuning the Composition of Electrodeposited Bimetallic Tin-Lead Catalysts for Enhanced Activity and Durability in Carbon Dioxide Electroreduction to Formate.

    Science.gov (United States)

    Moore, Colin E; Gyenge, Előd L

    2017-09-11

    Bimetallic Sn-Pb catalysts with five different Sn/Pb atomic ratios were electrodeposited on Teflonated carbon paper and non-Teflonated carbon cloth using both fluoroborate- and oxide-containing deposition media to produce catalysts for the electrochemical reduction of CO 2 (ERC) to formate (HCOO - ). The interaction between catalyst composition, morphology, substrate, and deposition media was investigated by using cyclic voltammetry and constant potential electrolysis at -2.0 V versus Ag/AgCl for 2 h in 0.5 m KHCO 3 . The catalysts were analyzed before and after electrolysis by using SEM and XRD to determine the mechanisms of Faradaic efficiency loss and degradation. Catalysts that are mainly Sn with 15-35 at % Pb generated Faradaic efficiencies up to 95 % with a stable performance. However, pure Sn catalysts showed high initial stage formate production rates but experienced an extensive (up to 30 %) decrease of the Faradaic efficiency. The XRD results demonstrated the presence of polycrystalline SnO 2 after electrolysis using Sn-Pb catalysts with 35 at % Pb and its absence in the case of pure Sn. It is proposed that the presence of Pb (15-35 at %) in mainly Sn catalysts stabilized SnO 2 , which is responsible for the enhanced Faradaic efficiency and catalytic durability in the ERC. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Application of sodium carbonate prevents sulphur poisoning of catalysts in automated total mercury analysis

    Science.gov (United States)

    McLagan, David S.; Huang, Haiyong; Lei, Ying D.; Wania, Frank; Mitchell, Carl P. J.

    2017-07-01

    Analysis of high sulphur-containing samples for total mercury content using automated thermal decomposition, amalgamation, and atomic absorption spectroscopy instruments (USEPA Method 7473) leads to rapid and costly SO2 poisoning of catalysts. In an effort to overcome this issue, we tested whether the addition of powdered sodium carbonate (Na2CO3) to the catalyst and/or directly on top of sample material increases throughput of sulphur-impregnated (8-15 wt%) activated carbon samples per catalyst tube. Adding 5 g of Na2CO3 to the catalyst alone only marginally increases the functional lifetime of the catalyst (31 ± 4 g of activated carbon analyzed per catalyst tube) in relation to unaltered catalyst of the AMA254 total mercury analyzer (17 ± 4 g of activated carbon). Adding ≈ 0.2 g of Na2CO3 to samples substantially increases (81 ± 17 g of activated carbon) catalyst life over the unaltered catalyst. The greatest improvement is achieved by adding Na2CO3 to both catalyst and samples (200 ± 70 g of activated carbon), which significantly increases catalyst performance over all other treatments and enables an order of magnitude greater sample throughput than the unaltered samples and catalyst. It is likely that Na2CO3 efficiently sequesters SO2, even at high furnace temperatures to produce Na2SO4 and CO2, largely negating the poisonous impact of SO2 on the catalyst material. Increased corrosion of nickel sampling boats resulting from this methodological variation is easily resolved by substituting quartz boats. Overall, this variation enables an efficient and significantly more affordable means of employing automated atomic absorption spectrometry instruments for total mercury analysis of high-sulphur matrices.

  13. Improving the stability and ethanol electro-oxidation activity of Pt catalysts by selectively anchoring Pt particles on carbon-nanotubes-supported-SnO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Li, J.J.; Wang, J.S.; Zhao, J.H.; Song, C.Y.; Wang, L.C. [School of Chemical Engineering and Energy, Zhengzhou University, Zhengzhou (China); Guo, X. [Department of Chemistry, Tsinghua University, Beijing (China)

    2012-10-15

    To improve the stability and activity of Pt catalysts for ethanol electro-oxidation, Pt nanoparticles were selectively deposited on carbon-nanotubes (CNTs)-supported-SnO{sub 2} to prepare Pt/SnO{sub 2}/CNTs and Pt/CNTs was prepared by impregnation method for reference study. X-ray diffraction (XRD) was used to confirm the crystalline structures of Pt/SnO{sub 2}/CNTs and Pt/CNTs. The stabilities of Pt/SnO{sub 2}/CNTs and Pt/CNTs were compared by analyzing the Pt size increase amplitude using transmission electron microscopy (TEM) images recorded before and after cyclic voltammetry (CV) sweeping. The results showed that the Pt size increase amplitude is evidently smaller for Pt/SnO{sub 2}/CNTs, indicating the higher stability of Pt/SnO{sub 2}/CNTs. Although both catalysts exhibit degradation of electrochemical active surface area (EAS) after CV sweeping, the EAS degradation for the former is lower, further confirming the higher stability of Pt/SnO{sub 2}/CNTs. CV and potentiostatic current-time curves were recorded for ethanol electro-oxidation on both catalysts before and after CV sweeping and the results showed that the mass specific activity of Pt/CNTs increases more than that of Pt/SnO{sub 2}/CNTs, indicating that Pt/CNTs experiences more severe evolution and is less stable. The calculated area specific activity of Pt/SnO{sub 2}/CNTs is larger than that of Pt/CNTs, indicating SnO{sub 2} can co-catalyze Pt due to plenty of interfaces between SnO{sub 2} and Pt. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  14. Physicochemical investigations of carbon nanofiber supported Cu/ZrO2 catalyst

    International Nuclear Information System (INIS)

    Din, Israf Ud; Shaharun, Maizatul S.; Subbarao, Duvvuri; Naeem, A.

    2014-01-01

    Zirconia-promoted copper/carbon nanofiber catalysts (Cu‐ZrO 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 3 ). The CNF activated with 5% HNO 3 produced higher surface area which is 155 m 2 /g. The catalyst was characterized by X-ray Diffraction (XRD), Fourier Transform Infra-Red (FTIR) and N 2 adsorption-desorption. The results showed that increase of HNO 3 concentration reduced the surface area and porosity of the catalyst

  15. Tethered catalysts for the hydration of carbon dioxide

    Science.gov (United States)

    Valdez, Carlos A; Satcher, Jr., Joe H; Aines, Roger D; Wong, Sergio E; Baker, Sarah E; Lightstone, Felice C; Stolaroff, Joshuah K

    2014-11-04

    A system is provided that substantially increases the efficiency of CO.sub.2 capture and removal by positioning a catalyst within an optimal distance from the air-liquid interface. The catalyst is positioned within the layer determined to be the highest concentration of carbon dioxide. A hydrophobic tether is attached to the catalyst and the hydrophobic tether modulates the position of the catalyst within the liquid layer containing the highest concentration of carbon dioxide.

  16. Magnetic properties of carbon nanotubes with and without catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Lipert, Kamil; Ritschel, Manfred; Leonhardt, Albrecht; Krupskaya, Yulia; Buechner, Bernd; Klingeler, Ruediger, E-mail: k.lipert@ifw-dresden.d [Leibniz Institute for Solid State and Materials Research (IFW) Dresden (Germany)

    2010-01-01

    In this paper we report on the magnetic properties of single- and multiwalled carbon nanotubes synthesized using different chemical vapour deposition methods and with variety of catalyst materials (ferromagnetic Fe, FeCo and diamagnetic Re). Different methods yield carbon nanotubes with different morphologies and different quantity of residual catalyst material. Catalyst particles are usually encapsulated in the nanotubes and influence the magnetic respond of the samples. Varying ferromagnetic properties depending on the shape, size and type of catalyst are discussed in detail. The data are compared with M(H) characteristics of carbon nanotubes without catalysts and with nonmagnetic rhenium, as a reference.

  17. TiO2-anatase modified by carbon as the photo catalyst under visible light

    International Nuclear Information System (INIS)

    Morawski, A.W.; Janus, M.; Tryba, B.; Kalucki, K.; Tryba, B.; Inagaki, M.

    2006-01-01

    The photo-catalytic oxidation of phenol in water under a visible light over anatase-type titanium dioxide (Tytanpol A11, Poland), modified by carbon deposited via n-hexane carbonization, was investigated. The catalysts, which had small (0-0.2 mass%) and high (0.69-0.85 mass%) contents of carbon showed a little lower catalytic photo-activity than pristine TiO 2 . However, the catalyst with high content of carbon (0.85 mass%) gave almost 14-times lower turbidity in the phenol solution after the photo-catalyst sedimentation. These two factors depend on the carbon content and have an influence on the 'practical efficiency' of the catalysts. The 'practical efficiency' of the catalyst under visible light, calculated from these two factors, was therefore 14-times higher for the catalyst containing 0.85 mass% carbon (whereas for UV radiation, it was found to be lower - 0.2 mass% -; this is the result of a previous work). The surface modification of the catalyst with 0.85% carbon seemed to be stable under visible light. The deposition of carbon on TiO 2 by carbonization of n-hexane was supposed to lead to obtain the catalyst, which could be easily used in a water-treatment system under visible light. (authors)

  18. 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.

  19. Gasification of carbon deposits on catalysts and metal surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Figueiredo, J L

    1986-10-01

    'Coke' deposited on catalysts and reactor surfaces includes a variety of carbons of different structures and origins, their reactivities being conveniently assessed by Temperature Programmed Reaction (TPR). The gasification of carbon deposits obtained in the laboratory under well controlled conditions, and the regeneration of coked catalysts from petroleum refining processes are reviewed and discussed. Filamentary carbon deposits, containing dispersed metal particles, behave as supported metal catalysts during gasification, and show high reactivities. Pyrolytic and acid catalysis carbons are less reactive on their own, as the gasification is not catalysed; however, metal components of the catalyst or metal impurities deposited on the surface may enhance gasification. 26 refs., 8 figs., 2 tabs.

  20. The role of Ni in sulfided carbon-supported Ni-Mo hydrodesulfurization catalysts

    NARCIS (Netherlands)

    Bouwens, S.M.A.M.; Barthe-Zahir, N.; Beer, de V.H.J.; Prins, R.

    1991-01-01

    The thiophene hydrodesulfurization activities of Ni and Ni---Mo sulfide catalysts supported on activated carbon were measured at atmospheric pressure and the catalyst structures were studied by means of X-ray photoelectron spectroscopy, dynamic oxygen chemisorption, and chemical sulfur analysis. The

  1. 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.

  2. THE EFFECT OF WATER CAPACITY ON THE ACTIVITY OF PD(II-CU(II CATALYST ANCHORED TO ACID-MODIFIED CLINOPTILOLITE IN THE REACTION OF LOW-TEMPERATURE CARBON MONOXIDE OXIDATION

    Directory of Open Access Journals (Sweden)

    T. L. Rakitskaya

    2015-02-01

    Full Text Available The maximum activity of Pd(II-Cu(II catalyst anchored to acid modified clinoptilolite in the reaction of low-temperature carbon monoxide oxidation with air oxygen has been found at the water content in the range from 3.3 to 4.2 mmol/g.

  3. Composite catalyst for carbon monoxide and hydrocarbon oxidation

    Science.gov (United States)

    Liu, Wei; Flytzani-Stephanopoulos, Maria

    1996-01-01

    A method and composition for the complete oxidation of carbon monoxide and/or hydrocarbon compounds. The method involves reacting the carbon monoxide and/or hydrocarbons with an oxidizing agent in the presence of a metal oxide composite catalyst. The catalyst is prepared by combining fluorite-type oxygen ion conductors with active transition metals. The fluorite oxide, selected from the group consisting of cerium oxide, zirconium oxide, thorium oxide, hafnium oxide, and uranium oxide, and may be doped by alkaline earth and rare earth oxides. The transition metals, selected from the group consisting of molybdnum, copper, cobalt, maganese, nickel, and silver, are used as additives. The atomic ratio of transition metal to fluorite oxide is less than one.

  4. Catalyst design for carbon nanotube growth using atomistic modeling

    International Nuclear Information System (INIS)

    Pint, Cary L; Bozzolo, Guillermo; Hauge, Robert

    2008-01-01

    The formation and stability of bimetallic catalyst particles, in the framework of carbon nanotube growth, is studied using the Bozzolo-Ferrante-Smith (BFS) method for alloys. Monte Carlo-Metropolis simulations with the BFS method are utilized in order to predict and study equilibrium configurations for nanoscale catalyst particles which are directly relevant to the catalyst state prior to growth of carbon nanotubes. At the forefront of possible catalyst combinations is the popular Fe-Mo bimetallic catalyst, which we have recently studied experimentally. We explain our experimental results, which indicate that the growth observed is dependent on the order of co-catalyst deposition, in the straightforward interpretation of BFS strain and chemical energy contributions toward the formation of Fe-Mo catalyst prior to growth. We find that the competition between the formation of metastable inner Mo cores and clusters of surface-segregated Mo atoms in Fe-Mo catalyst particles influences catalyst formation, and we investigate the role of Mo concentration and catalyst particle size in this process. Finally, we apply the same modeling approach to other prominent bimetallic catalysts and suggest that this technique can be a powerful tool to understand and manipulate catalyst design for highly efficient carbon nanotube growth

  5. Effect of P on the electrochemical activity of carbon supported Pt-Ru alloy catalyst for methanol oxidation.

    CSIR Research Space (South Africa)

    Mohlala, M

    2007-11-01

    Full Text Available for direct alcohol fuel cell is lower than that of the hydrogen PEMFC [3, 4, and 5]. This study aims at improving the performance of the binary catalyst through the addition of phosphorus group following the sodium hypophosphite method [6]. The optimum amount...

  6. Catalyst retention in continuous flow with supercritical carbon dioxide

    NARCIS (Netherlands)

    Stouten, S.C.; Noel, T.; Wang, Q.; Hessel, V.

    2014-01-01

    This review discusses the retention of organometallic catalysts in continuous flow processes utilizing supercritical carbon dioxide. Due to its innovative properties, supercritical carbon dioxide offers interesting possibilities for process intensification. As a result of safety and cost

  7. Effects of calcination and activation conditions on ordered mesoporous carbon supported iron catalysts for production of lower olefins from synthesis gas

    NARCIS (Netherlands)

    Oschatz, M; van Deelen, T W; Weber, J L; Lamme, W S; Wang, G; Goderis, B; Verkinderen, O; Dugulan, A I; de Jong, K P

    2016-01-01

    Lower C2–C4 olefins are important commodity chemicals usually produced by steam cracking of naphtha or fluid catalytic cracking of vacuum gas oil. The Fischer–Tropsch synthesis of lower olefins (FTO) with iron-based catalysts uses synthesis gas as an alternative feedstock. Nanostructured carbon

  8. Enhanced life of proton exchange membrane fuel cell catalysts using perfluorosulfonic acid stabilized carbon support

    International Nuclear Information System (INIS)

    Cheng Niancai; Mu Shichun; Chen Xiaojing; Lv Haifeng; Pan Mu; Edwards, Peter P.

    2011-01-01

    We report a new and simple solution to increase life of Pt/C catalysts using the proton-conducting polymer (perfluorosulfonic acid, PFSA) stabilized carbon support (denoted these catalysts as Pt/NFC catalysts) as compared to conventional Pt/C catalysts commonly used in PEM fuel cells. A high catalytic activity of the catalyst is observed by both CV (cyclic voltammetry) and ORR (oxygen reduction reaction) measurements. Especially, our own catalysts have a 60% better life as compared to Pt/C under electrochemically accelerated durability test conditions. The loss rate of electrochemical active area (ECA) for Pt/NFC catalysts is only 0.007 m 2 g -1 cycle -1 , compared to a value of 0.011 m 2 g -1 cycle -1 for Pt/C.

  9. Enhanced life of proton exchange membrane fuel cell catalysts using perfluorosulfonic acid stabilized carbon support

    Energy Technology Data Exchange (ETDEWEB)

    Cheng Niancai [State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070 (China); Mu Shichun, E-mail: msc@whut.edu.c [State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070 (China); Department of Chemistry, Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, OX1 3QR (United Kingdom); Chen Xiaojing; Lv Haifeng; Pan Mu [State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070 (China); Edwards, Peter P. [Department of Chemistry, Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, OX1 3QR (United Kingdom)

    2011-02-01

    We report a new and simple solution to increase life of Pt/C catalysts using the proton-conducting polymer (perfluorosulfonic acid, PFSA) stabilized carbon support (denoted these catalysts as Pt/NFC catalysts) as compared to conventional Pt/C catalysts commonly used in PEM fuel cells. A high catalytic activity of the catalyst is observed by both CV (cyclic voltammetry) and ORR (oxygen reduction reaction) measurements. Especially, our own catalysts have a 60% better life as compared to Pt/C under electrochemically accelerated durability test conditions. The loss rate of electrochemical active area (ECA) for Pt/NFC catalysts is only 0.007 m{sup 2} g{sup -1} cycle{sup -1}, compared to a value of 0.011 m{sup 2} g{sup -1} cycle{sup -1} for Pt/C.

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

    International Nuclear Information System (INIS)

    Park, Eunsil; Kim, Jongwon; Lee, Changseop

    2014-01-01

    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 2 g -1 high specific surface area

  11. Activation of heterogenised rhodium carbonylation catalyst infrared spectroscopic study

    Energy Technology Data Exchange (ETDEWEB)

    Scurrell, M S

    1977-01-01

    In a study related to heterogeneous versions of homogeneous catalysts active in carbonylation of methanol to acetic acid, the catalyst consisted of 1Vertical Bar3< rhodium as rhodium trichloride supported on 13X zeolite and evacuated at 437/sup 0/K. Contacting the catalyst with carbon monoxide caused two bands, at 2025 and 2095 cm/sup -1/, to appear. Contact with a mixture of carbon monoxide and methyl iodide (the usual promoter) caused bands at 2085, 1710, 1440, and 1370 cm/sup -1/ to appear; the first two correspond to the bands at 2062 and 1711 cm/sup -1/ in homogeneous catalysts attributed to the formation of Rh(CH/sup 3/CO)(CO)X/sup 2/I/sup -/. Spectra.

  12. Elucidating the Origin of Hydrogen Evolution Reaction Activity in Mono- and Bimetallic Metal- and Nitrogen-Doped Carbon Catalysts (Me-N-C).

    Science.gov (United States)

    Shahraei, Ali; Moradabadi, Ashkan; Martinaiou, Ioanna; Lauterbach, Stefan; Klemenz, Sebastian; Dolique, Stephanie; Kleebe, Hans-Joachim; Kaghazchi, Payam; Kramm, Ulrike I

    2017-08-02

    In this work, we present a comprehensive study on the role of metal species in MOF-based Me-N-C (mono- and bimetallic) catalysts for the hydrogen evolution reaction (HER). The catalysts are investigated with respect to HER activity and stability in alkaline electrolyte. On the basis of the structural analysis by X-ray diffraction, X-ray-induced photoelectron spectroscopy, and transmission electron microscopy, it is concluded that MeN 4 sites seem to dominate the HER activity of these catalysts. There is a strong relation between the amount of MeN 4 sites that are formed and the energy of formation related to these sites integrated at the edge of a graphene layer, as obtained from density functional theory (DFT) calculations. Our results show, for the first time, that the combination of two metals (Co and Mo) in a bimetallic (Co,Mo)-N-C catalyst allows hydrogen production with a significantly improved overpotential in comparison to its monometallic counterparts and other Me-N-C catalysts. By the combination of experimental results with DFT calculations, we show that the origin of the enhanced performance of our (Co,Mo)-N-C catalyst seems to be provided by an improved hydrogen binding energy on one MeN 4 site because of the presence of a second MeN 4 site in its close vicinity, as investigated in detail for our most active (Co,Mo)-N-C catalyst. The outstanding stability and good activity make especially the bimetallic Me-N-C catalysts interesting candidates for solar fuel applications.

  13. Metal Nanoparticle Catalysts for Carbon Nanotube Growth

    Science.gov (United States)

    Pierce, Benjamin F.

    2003-01-01

    Work this summer involved and new and unique process for producing the metal nanoparticle catalysts needed for carbon nanotube (CNT) growth. There are many applications attributed to CNT's, and their properties have deemed them to be a hot spot in research today. Many groups have demonstrated the versatility in CNT's by exploring a wide spectrum of roles that these nanotubes are able to fill. A short list of such promising applications are: nanoscaled electronic circuitry, storage media, chemical sensors, microscope enhancement, and coating reinforcement. Different methods have been used to grow these CNT's. Some examples are laser ablation, flame synthesis, or furnace synthesis. Every single approach requires the presence of a metal catalyst (Fe, Co, and Ni are among the best) that is small enough to produce a CNT. Herein lies the uniqueness of this work. Microemulsions (containing inverse micelles) were used to generate these metal particles for subsequent CNT growth. The goal of this summer work was basically to accomplish as much preliminary work as possible. I strived to pinpoint which variable (experimental process, metal product, substrate, method of application, CVD conditions, etc.) was the determining factor in the results. The resulting SEM images were sufficient for the appropriate comparisons to be made. The future work of this project consists of the optimization of the more promising experimental procedures and further exploration onto what exactly dictated the results.

  14. 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.

  15. Improvement of activated carbons as oxygen reduction catalysts in neutral solutions by ammonia gas treatment and their performance in microbial fuel cells

    KAUST Repository

    Watson, Valerie J.

    2013-11-01

    Commercially available activated carbon (AC) powders from different precursor materials (peat, coconut shell, coal, and hardwood) were treated with ammonia gas at 700 C to improve their performance as oxygen reduction catalysts in neutral pH solutions used in microbial fuel cells (MFCs). The ammonia treated ACs exhibited better catalytic performance in rotating ring-disk electrode tests than their untreated precursors, with the bituminous based AC most improved, with an onset potential of Eonset = 0.12 V (untreated, Eonset = 0.08 V) and n = 3.9 electrons transferred in oxygen reduction (untreated, n = 3.6), and the hardwood based AC (treated, E onset = 0.03 V, n = 3.3; untreated, Eonset = -0.04 V, n = 3.0). Ammonia treatment decreased oxygen content by 29-58%, increased nitrogen content to 1.8 atomic %, and increased the basicity of the bituminous, peat, and hardwood ACs. The treated coal based AC cathodes had higher maximum power densities in MFCs (2450 ± 40 mW m-2) than the other AC cathodes or a Pt/C cathode (2100 ± 1 mW m-2). These results show that reduced oxygen abundance and increased nitrogen functionalities on the AC surface can increase catalytic performance for oxygen reduction in neutral media. © 2013 Elsevier B.V. All rights reserved.

  16. Application of aromatization catalyst in synthesis of carbon nanotubes

    Indian Academy of Sciences (India)

    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 ...

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

    NARCIS (Netherlands)

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

  18. Sulfidation of carbon-supported iron oxide catalysts

    NARCIS (Netherlands)

    Ramselaar, W.L.T.M.; Hadders, R.H.; Gerkema, E.; Beer, de V.H.J.; Oers, van E.M.; Kraan, van der A.M.

    1989-01-01

    The sulfidation of carbon-supported iron oxide catalysts was studied by means of in-situ Mössbauer spectroscopy at temperatures down to 4.2 K. The catalysts were dried in two different ways and then sulfided in a flow of 10% H2S in H2 at temperatures between 293 and 773 K. Thiophene

  19. Synthesis of 2D Nitrogen-Doped Mesoporous Carbon Catalyst for Oxygen Reduction Reaction

    Directory of Open Access Journals (Sweden)

    Zhipeng Yu

    2017-02-01

    Full Text Available 2D nitrogen-doped mesoporous carbon (NMC is synthesized by using a mesoporous silica film as hard template, which is then investigated as a non-precious metal catalyst for the oxygen reduction reaction (ORR. The effect of the synthesis conditions on the silica template and carbon is extensively investigated. In this work, we employ dual templates—viz. graphene oxide and triblock copolymer F127—to control the textural features of a 2D silica film. The silica is then used as a template to direct the synthesis of a 2D nitrogen-doped mesoporous carbon. The resultant nitrogen-doped mesoporous carbon is characterized by transmission electron microscopy (TEM, nitrogen ad/desorption isotherms, X-ray photoelectron spectroscopy (XPS, cyclic voltammetry (CV, and rotating disk electrode measurements (RDE. The electrochemical test reveals that the obtained 2D-film carbon catalyst yields a highly electrochemically active surface area and superior electrocatalytic activity for the ORR compared to the 3D-particle. The superior activity can be firstly attributed to the difference in the specific surface area of the two catalysts. More importantly, the 2D-film morphology makes more active sites accessible to the reactive species, resulting in a much higher utilization efficiency and consequently better activity. Finally, it is noted that all the carbon catalysts exhibit a higher ORR activity than a commercial Pt catalyst, and are promising for use in fuel cells.

  20. Visible light photocatalytic activities of template free porous graphitic carbon nitride-BiOBr composite catalysts towards the mineralization of reactive dyes

    Science.gov (United States)

    Kanagaraj, Thamaraiselvi; Thiripuranthagan, Sivakumar; Paskalis, Sahaya Murphin Kumar; Abe, Hideki

    2017-12-01

    Template free porous g-C3N4 (pGCN) and flower like bismuth oxybromide catalysts were synthesized by poly condensation and precipitation methods respectively. Various weight percentages of porous GCN-BiOBr composite catalysts (x% pGCN-BiOBr where x = 5, 10, 30, 50 & 70 wt% of pGCN) were synthesized by impregnation method. All the synthesized catalysts were characterized by X-Ray diffractometer, Fourier transform infrared spectrophotometer, BET surface area analyzer, UV Visible diffuse reflectance spectrophotometer, X-Ray photoelectron spectrophotometer, SEM with Energy dispersive X-ray analyzer (SEM/EDAX) and elemental mapping, Transmission electron microscope, Photoluminescence spectrophotometer and Electrochemical impedance. Photocatalytic degradation of all the synthesized catalysts were tested towards the harmful reactive dyes such as reactive blue 198 (RB 198), reactive black 5 (RB 5) and reactive yellow 145 (RY 145) in presence of visible irradiation. Among the catalysts 30% pGCN-BiOBr resulted in the highest photocatalytic activity towards the degradation of all the three dyes in presence of UV, visible and solar irradiations. Kinetics studies on the photocatalytic mineralization of dyes indicated that it followed pseudo first order. HPLC, TOC and COD studies confirm that the dyes are mineralized into CO2, water and mineral salts.

  1. Biodiesel production from Silybum marianum L. seed oil with high FFA content using sulfonated carbon catalyst for esterification and base catalyst for transesterification

    International Nuclear Information System (INIS)

    Fadhil, Abdelrahman B.; Aziz, Akram M.; Al-Tamer, Marwa H.

    2016-01-01

    Highlights: • PET was converted to activated carbon and then sulfonated to prepare carbon acid catalyst. • Carbon acid catalyst was used for esterification of high acid value Silybum marianum L. seed oil. • Biodiesel was obtained with 96.98% efficiency. - Abstract: In this research work, waste of polyethylene terephthalate (PET) was converted into activated carbon and the latter was used in the preparation of a carbon acid catalyst. Waste of PET was converted into activated carbon via carbonization and steam activation, then the activated carbon was sulfonated using fuming sulfuric acid in order to produce the carbon acid catalyst. The prepared carbon acid catalyst was tested for esterification of high acid value non-edible oil, Silybum marianum L. seed oil (SMSO) via optimized protocol. Amount of the carbon acid catalyst, methanol to oil molar ratio, temperature and time were the experimental variables optimized. Esterification of SMSO with methanol using the prepared carbon acid catalyst reduced its parent acid value (20.0 mg KOH/g) to the acceptable limits for base-catalyzed transesterification (<2.0 mg KOH/g) using 6.0% w/w of the catalyst, 15:1 methanol to oil molar ratio, 68 °C reaction temperature and 180 min of reaction. The performance of the catalyst was reduced gradually during its recycling and reached to 60.0% at the 5th cycle. Kinetics of esterification of SMSO using the prepared carbon acid catalyst followed pseudo first order kinetics, and the activation energy was found to be 70.98 kJ/mol. The esterified oil was converted to biodiesel through optimized base-catalyzed transesterification with methanol. Biodiesel with (96.98% yield and purity of 96.69% w/w) yield was obtained using 0.80% KOH w/w, 6:1 methanol to oil molar ratio, 60 °C reaction temperature, 75 min of reaction and 600 rpm rate of stirring. The biodiesel properties were within the recommended biodiesel standards as prescribed by ASTM D 6751 and EN 14214. Transesterification of

  2. 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.

  3. Highly Stable and Active Catalyst for Sabatier Reactions

    Science.gov (United States)

    Hu, Jianli; Brooks, Kriston P.

    2012-01-01

    Highly active Ru/TiO2 catalysts for Sabatier reaction have been developed. The catalysts have shown to be stable under repeated shutting down/startup conditions. When the Ru/TiO2 catalyst is coated on the engineered substrate Fe-CrAlY felt, activity enhancement is more than doubled when compared with an identically prepared engineered catalyst made from commercial Degussa catalyst. Also, bimetallic Ru-Rh/TiO2 catalysts show high activity at high throughput.

  4. Functionalized Natural Carbon-Supported Nanoparticles as Excellent Catalysts for Hydrocarbon Production.

    Science.gov (United States)

    Sun, Jian; Guo, Lisheng; Ma, Qingxiang; Gao, Xinhua; Yamane, Noriyuki; Xu, Hengyong; Tsubaki, Noritatsu

    2017-02-01

    We report a one-pot and eco-friendly synthesis of carbon-supported cobalt nanoparticles, achieved by carbonization of waste biomass (rice bran) with a cobalt source. The functionalized biomass provides carbon microspheres as excellent catalyst support, forming a unique interface between hydrophobic and hydrophilic groups. The latter, involving hydroxyl and amino groups, can catch much more active cobalt nanoparticles on surface for Fischer-Tropsch synthesis than chemical carbon. The loading amount of cobalt on the final catalyst is much higher than that prepared with a chemical carbon source, such as glucose. The proposed concept of using a functionalized natural carbon source shows great potential compared with conventional carbon sources, and will be meaningful for other fields concerning carbon support, such as heterogeneous catalysis or electrochemical fields. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  5. Effect of preparation method on catalytic activity of Ni/ γ-Al2O3 catalysts

    International Nuclear Information System (INIS)

    Miranda Morales, Barbara

    2017-01-01

    The performance of catalysts was shown to be strongly dependent on their methods of preparation. A study to examine the relationship between catalyst preparation procedures and the structure, dispersion, activity, and selectivity of the finished catalyst is reported. 10 wt.%Ni/γ-Al 2 O 3 catalysts were prepared by incipient wetness impregnation and by wet impregnation. The catalysts were used in the conversion of glycerol in gas phase and atmospheric pressure. The selectivity and activity of the catalysts were affected by the preparation method employed. The catalysts were characterized by thermogravimetric analysis (TGA), temperature-programmed reduction (TPR), N 2 -physorption, H 2 -chemisorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FTIR) and temperature-programmed oxidation (TPO). The Ni particle size and dispersion of the catalysts affected the selectivity to hydrogenolysis and dehydration routes, and the formation of carbon deposits was also affected. (author) [es

  6. Effect of preparation method on the surface characteristics and activity of the Pd/OMS-2 catalysts for the oxidation of carbon monoxide, toluene, and ethyl acetate

    Science.gov (United States)

    Liu, Lisha; Song, Yong; Fu, Zhidan; Ye, Qing; Cheng, Shuiyuan; Kang, Tianfang; Dai, Hongxing

    2017-02-01

    The cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2)-supported Pd (0.5 wt% Pd/OMS-2-DP, 0.5 wt% Pd/OMS-2-PI, and 0.5 wt% Pd/OMS-2-EX) catalysts were prepared by the deposition-precipitation, pre-incorporation, and ion-exchanging strategies, respectively. It is shown that the preparation method exerted an important effect on the physicochemical property of the sample. Among the OMS-2-supported Pd catalysts, 0.5 wt% Pd/OMS-2-DP possessed the highest surface (Mn2+ + Mn3+)/Mn4+ atomic ratio and the highest surface Pd loading and acid sites. The 0.5 wt% Pd/OMS-2 catalysts outperformed the Pd-free counterpart, among which 0.5 wt% Pd/OMS-2-DP presented the best catalytic activity (T50% and T90% were 25 and 55 °C for CO oxidation, 240 and 285 °C for toluene oxidation, and 160 and 200 °C for ethyl acetate oxidation, respectively). We believe that the high Pd surface loading, high surface atomic ratio of (Mn2+ + Mn3+)/Mn4+, and good low-temperature reducibility, good oxygen mobility, and high acidity were responsible for the excellent performance of the 0.5 wt% Pd/OMS-2-DP catalyst.

  7. Carbon nanocages: a new support material for Pt catalyst with remarkably high durability.

    Science.gov (United States)

    Wang, Xiao Xia; Tan, Zhe Hua; Zeng, Min; Wang, Jian Nong

    2014-03-24

    Low durability is the major challenge hindering the large-scale implementation of proton exchange membrane fuel cell (PEMFC) technology, and corrosion of carbon support materials of current catalysts is the main cause. Here, we describe the finding of remarkably high durability with the use of a novel support material. This material is based on hollow carbon nanocages developed with a high degree of graphitization and concurrent nitrogen doping for oxidation resistance enhancement, uniform deposition of fine Pt particles, and strong Pt-support interaction. Accelerated degradation testing shows that such designed catalyst possesses a superior electrochemical activity and long-term stability for both hydrogen oxidation and oxygen reduction relative to industry benchmarks of current catalysts. Further testing under conditions of practical fuel cell operation reveals almost no degradation over long-term cycling. Such a catalyst of high activity, particularly, high durability, opens the door for the next-generation PEMFC for "real world" application.

  8. Efficient Cycloaddition Reaction of Carbon Dioxide with Epoxide by Rhodamine Based Catalyst Under 1 atm Pressure

    Energy Technology Data Exchange (ETDEWEB)

    Gong, Qing; Luo, Huadong; Cao, Di; Zhang, Haibo; Wang, Wenjing; Zhou, Xiaohai [Wuhan University, Wuhan (China)

    2012-06-15

    Rhodamine B (RhB) and rhodamine 6G (Rh6G) were employed as catalysts for the synthesis of cyclic carbonate from carbon dioxide and epoxide. It turned out that the catalytic activity of Rh6G was nearly 29 times higher than that of RhB at 1 atm pressure, 90 .deg. C. Furthermore, the catalytic efficiency of RhB and Rh6G was greatly enhanced with triethylamine as co-catalyst. Under the optimized conditions, the best isolated yield (93%) of cyclic carbonate was achieved without organic solvent and metal component

  9. 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

  10. Catalyst deposition for the preparation of carbon nanotubes

    DEFF Research Database (Denmark)

    2013-01-01

    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....

  11. 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.

  12. Studies on recycling and utilization of spent catalysts. Preparation of active hydrodemetallization catalyst compositions from spent residue hydroprocessing catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Marafi, Meena; Stanislaus, Antony [Petroleum Refining Department, Petroleum Research and Studies Center, Kuwait Institute for Scientific Research, P.O. Box 24885, Safat (Kuwait)

    2007-02-15

    Spent catalysts form a major source of solid wastes in the petroleum refining industries. Due to environmental concerns, increasing emphasis has been placed on the development of recycling processes for the waste catalyst materials as much as possible. In the present study the potential reuse of spent catalysts in the preparation of active new catalysts for residual oil hydrotreating was examined. A series of catalysts were prepared by mixing and extruding spent residue hydroprocessing catalysts that contained C, V, Mo, Ni and Al{sub 2}O{sub 3} with boehmite in different proportions. All prepared catalysts were characterized by chemical analysis and by surface area, pore volume, pore size and crushing strength measurements. The hydrodesulfurization (HDS) and hydrodemetallization (HDM) activities of the catalysts were evaluated by testing in a high pressure fixed-bed microreactor unit using Kuwait atmospheric residue as feed. A commercial HDM catalyst was also tested under similar operating conditions and their HDS and HDM activities were compared with that of the prepared catalysts. The results revealed that catalyst prepared with addition of up to 40 wt% spent catalyst to boehmite had fairly high surface area and pore volume together with large pores. The catalyst prepared by mixing and extruding about 40 wt% spent catalyst with boehmite was relatively more active for promoting HDM and HDS reactions than a reference commercial HDM catalyst. The formation of some kind of new active sites from the metals (V, Mo and Ni) present in the spent catalyst is suggested to be responsible for the high HDM activity of the prepared catalyst. (author)

  13. Carbon in palladium catalysts: A metastable carbide

    International Nuclear Information System (INIS)

    Seriani, Nicola; Mittendorfer, Florian; Kresse, Georg

    2010-01-01

    The catalytic activity of palladium towards selective hydrogenation of hydrocarbons depends on the partial pressure of hydrogen. It has been suggested that the reaction proceeds selectively towards partial hydrogenation only when a carbon-rich film is present at the metal surface. On the basis of first-principles simulations, we show that carbon can dissolve into the metal because graphite formation is delayed by the large critical nucleus necessary for graphite nucleation. A bulk carbide Pd 6 C with a hexagonal 6-layer fcc-like supercell forms. The structure is characterized by core level shifts of 0.66-0.70 eV in the core states of Pd, in agreement with experimental x-ray photoemission spectra. Moreover, this phase traps bulk-dissolved hydrogen, suppressing the total hydrogenation reaction channel and fostering partial hydrogenation. (author)

  14. Activity and selectivity control through periodic composition forcing over Fischer-Tropsch catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Silveston, P L; Hudgins, R R; Adesina, A A; Ross, G S; Feimer, J L

    1986-01-01

    Data collected under steady-state and periodic composition forcing of the Fischer-Tropsch synthesis over three commonly used catalysts demonstrate that both activity and selectivity can be changed by the latter operating mode. Synthesis of hydrocarbons up to C/sub 7/are favored at the expense of the higher carbon numbers for the Co catalyst, while for the Ru catalyst, only the C/sub 3/ and lower species are favored. Only methane production is stimulated with the Fe catalyst. Fe and Ru catalysts shift production from alkenes to alkanes. Transient data is interpreted in the paper.

  15. Solar-Driven Hydrogen Peroxide Production Using Polymer-Supported Carbon Dots as Heterogeneous Catalyst

    Science.gov (United States)

    Gogoi, Satyabrat; Karak, Niranjan

    2017-10-01

    Safe, sustainable, and green production of hydrogen peroxide is an exciting proposition due to the role of hydrogen peroxide as a green oxidant and energy carrier for fuel cells. The current work reports the development of carbon dot-impregnated waterborne hyperbranched polyurethane as a heterogeneous photo-catalyst for solar-driven production of hydrogen peroxide. The results reveal that the carbon dots possess a suitable band-gap of 2.98 eV, which facilitates effective splitting of both water and ethanol under solar irradiation. Inclusion of the carbon dots within the eco-friendly polymeric material ensures their catalytic activity and also provides a facile route for easy catalyst separation, especially from a solubilizing medium. The overall process was performed in accordance with the principles of green chemistry using bio-based precursors and aqueous medium. This work highlights the potential of carbon dots as an effective photo-catalyst.

  16. Effect of preparation method on the surface characteristics and activity of the Pd/OMS-2 catalysts for the oxidation of carbon monoxide, toluene, and ethyl acetate

    International Nuclear Information System (INIS)

    Liu, Lisha; Song, Yong; Fu, Zhidan; Ye, Qing; Cheng, Shuiyuan; Kang, Tianfang; Dai, Hongxing

    2017-01-01

    Highlights: • The framework-structured of cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) has a 2 × 2 square tunnel. • Preparation route has an important impact on physicochemical property of the product. • Pd/OMS-2-DP via the deposition-precipitation route shows excellent catalytic activity. • Pd surface loading, surface atomic ratio of Mn ions, lattice oxygen mobility, oxygen vacancy, reducibility and acidity govern activity. - Abstract: The cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2)-supported Pd (0.5 wt% Pd/OMS-2-DP, 0.5 wt% Pd/OMS-2-PI, and 0.5 wt% Pd/OMS-2-EX) catalysts were prepared by the deposition-precipitation, pre-incorporation, and ion-exchanging strategies, respectively. It is shown that the preparation method exerted an important effect on the physicochemical property of the sample. Among the OMS-2-supported Pd catalysts, 0.5 wt% Pd/OMS-2-DP possessed the highest surface (Mn 2+ + Mn 3+ )/Mn 4+ atomic ratio and the highest surface Pd loading and acid sites. The 0.5 wt% Pd/OMS-2 catalysts outperformed the Pd-free counterpart, among which 0.5 wt% Pd/OMS-2-DP presented the best catalytic activity (T 50% and T 90% were 25 and 55 °C for CO oxidation, 240 and 285 °C for toluene oxidation, and 160 and 200 °C for ethyl acetate oxidation, respectively). We believe that the high Pd surface loading, high surface atomic ratio of (Mn 2+ + Mn 3+ )/Mn 4+ , and good low-temperature reducibility, good oxygen mobility, and high acidity were responsible for the excellent performance of the 0.5 wt% Pd/OMS-2-DP catalyst.

  17. Effect of preparation method on the surface characteristics and activity of the Pd/OMS-2 catalysts for the oxidation of carbon monoxide, toluene, and ethyl acetate

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Lisha; Song, Yong; Fu, Zhidan [Key Laboratory of Beijing on Regional Air Pollution Control, Department of Environmental Science, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China); Ye, Qing, E-mail: yeqing@bjut.edu.cn [Key Laboratory of Beijing on Regional Air Pollution Control, Department of Environmental Science, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China); Cheng, Shuiyuan; Kang, Tianfang [Key Laboratory of Beijing on Regional Air Pollution Control, Department of Environmental Science, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China); Dai, Hongxing, E-mail: hxdai@bjut.edu.cn [Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Department of Chemistry and Chemical Engineering, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China)

    2017-02-28

    Highlights: • The framework-structured of cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) has a 2 × 2 square tunnel. • Preparation route has an important impact on physicochemical property of the product. • Pd/OMS-2-DP via the deposition-precipitation route shows excellent catalytic activity. • Pd surface loading, surface atomic ratio of Mn ions, lattice oxygen mobility, oxygen vacancy, reducibility and acidity govern activity. - Abstract: The cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2)-supported Pd (0.5 wt% Pd/OMS-2-DP, 0.5 wt% Pd/OMS-2-PI, and 0.5 wt% Pd/OMS-2-EX) catalysts were prepared by the deposition-precipitation, pre-incorporation, and ion-exchanging strategies, respectively. It is shown that the preparation method exerted an important effect on the physicochemical property of the sample. Among the OMS-2-supported Pd catalysts, 0.5 wt% Pd/OMS-2-DP possessed the highest surface (Mn{sup 2+} + Mn{sup 3+})/Mn{sup 4+} atomic ratio and the highest surface Pd loading and acid sites. The 0.5 wt% Pd/OMS-2 catalysts outperformed the Pd-free counterpart, among which 0.5 wt% Pd/OMS-2-DP presented the best catalytic activity (T{sub 50%} and T{sub 90%} were 25 and 55 °C for CO oxidation, 240 and 285 °C for toluene oxidation, and 160 and 200 °C for ethyl acetate oxidation, respectively). We believe that the high Pd surface loading, high surface atomic ratio of (Mn{sup 2+} + Mn{sup 3+})/Mn{sup 4+}, and good low-temperature reducibility, good oxygen mobility, and high acidity were responsible for the excellent performance of the 0.5 wt% Pd/OMS-2-DP catalyst.

  18. Temperature-programmed reduction and cyclic voltammetry of Pt/carbon-fibre paper catalysts for methanol electrooxidation

    International Nuclear Information System (INIS)

    Attwood, P.A.; McNicol, B.D.; Short, R.T.

    1981-01-01

    Temperature-programmed reduction (TPR) and cyclic voltammetry (CV) studies of platinum catalysts supported on pyrographite-coated carbon-fibre paper, and prepared by either ion exchange or impregnation, clearly demonstrate the nature of the interactions between the platinum species and the support. After drying the above catalysts at 120 0 C, the ion-exchanged preparation exhibits the stronger interaction with the carbon support, as might be expected since a chemical interaction with carbon surface groups is known to occur in such catalysts. The presence of a fraction of bulk Pt(NH 3 ) 4 (OH) 2 impregnating salt in the impregnated catalyst has been detected using TPR. After air activation at 300 0 C, subambient reduction peaks were observed and the strength of binding of Pt in the ion-exchanged catalyst was reflected by its increased difficulty of reduction in comparison with that of the impregnated catalyst. The stoichiometry of reduction in ion-exchanged catalysts corresponds to Pt 2+ → Pt 0 in both dried and activated catalysts, with a small amount of Pt 4+ present in the latter. Upon activation the impregnated catalyst showed the presence of some Pt metal, which was thought to arise from the decomposition of the fraction of bulk Pt(NH 3 ) 4 (OH) 2 in the dried catalyst. Activation of ion-exchanged catalysts at temperatures higher than 300 0 C led to a progressive weakening of the Pt-support interaction and consequent smaller Pt surface areas. Activation at 500 0 C in air produced Pt metal exclusively and very low Pt surface areas. The strong interaction between Pt and the carbon support upon activation of the ion-exchanged catalyst at 300 0 C is thought to be the origin of the large metal surface area and the high catalytic activity for methanol electrooxidation found upon reduction

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

    Directory of Open Access Journals (Sweden)

    Cinthia Alegre

    2015-03-01

    Full Text Available 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-ray diffraction and transmission electron microscopy were applied. Cyclic voltammetry and chronoamperometry were used for studying carbon monoxide and methanol oxidation. Catalysts supported on carbon xerogel presented higher catalytic activities towards CO and CH3OH oxidation than catalysts supported on Vulcan. The higher mesoporosity of carbon xerogel was responsible for the favored diffusion of reagents towards catalytic centers.

  20. 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.)

  1. Pulsed laser dewetting of nickel catalyst for carbon nanofiber growth

    International Nuclear Information System (INIS)

    Guan, Y F; Pearce, R C; Simpson, M L; Rack, P D; Melechko, A V; Hensley, D K

    2008-01-01

    We present a pulsed laser dewetting technique that produces single nickel catalyst particles from lithographically patterned disks for subsequent carbon nanofiber growth through plasma enhanced chemical vapor deposition. Unlike the case for standard heat treated Ni catalyst disks, for which multiple nickel particles and consequently multiple carbon nanofibers (CNFs) are observed, single vertically aligned CNFs could be obtained from the laser dewetted catalyst. Different laser dewetting parameters were tested in this study, such as the laser energy density and the laser processing time measured by the total number of laser pulses. Various nickel disk radii and thicknesses were attempted and the resultant number of carbon nanofibers was found to be a function of the initial disk dimension and the number of laser pulses

  2. Carbon catalysts for electrochemical hydrogen peroxide production in acidic media

    DEFF Research Database (Denmark)

    Čolić, Viktor; Yang, Sungeun; Révay, Zsolt

    2018-01-01

    Hydrogen peroxide is a commodity chemical, as it is an environmentally friendly oxidant. The electrochemical production of H2O2 from oxygen and water by the reduction of oxygen is of great interest, as it would allow the decentralized, on-site, production of pure H2O2. The ability to run...... the reaction in an acidic electrolyte with high performance is particularly important, as it would allow the use of polymer solid electrolytes and the production of pH-neutral hydrogen peroxide. Carbon catalysts, which are cheap, abundant, durable and can be highly selective show promise as potential catalysts...... for such systems. In this work, we examine the electrocatalytic performance and properties of seven commercially available carbon materials for H2O2 production by oxygen electroreduction. We show that the faradaic efficiencies for the reaction lie in a wide range of 18-82% for different carbon catalysts. In order...

  3. 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.

  4. Highly active carbon supported ternary PdSnPtx (x=0.1-0.7) catalysts for ethanol electro-oxidation in alkaline and acid media.

    Science.gov (United States)

    Wang, Xiaoguang; Zhu, Fuchun; He, Yongwei; Wang, Mei; Zhang, Zhonghua; Ma, Zizai; Li, Ruixue

    2016-04-15

    A series of trimetallic PdSnPtx (x=0.1-0.7)/C catalysts with varied Pt content have been synthesized by co-reduction method using NaBH4 as a reducing agent. These catalysts were characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), energy dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS), cyclic voltammetry (CV) and chronoamperometry (CA). The electrochemical results show that, after adding a minor amount of Pt dopant, the resultant PdSnPtx/C demonstrated more superior catalytic performance toward ethanol oxidation as compared with that of mono-/bi-metallic Pd/C or PdSn/C in alkaline solution and the PdSnPt0.2/C with optimal molar ratio reached the best. In acid solution, the PdSnPt0.2/C also depicted a superior catalytic activity relative to the commercial Pt/C catalyst. The possible enhanced synergistic effect between Pd, Sn/Sn(O) and Pt in an alloyed state should be responsible for the as-revealed superior ethanol electro-oxidation performance based upon the beneficial electronic effect and bi-functional mechanism. It implies the trimetallic PdSnPt0.2/C with a low Pt content has a promising prospect as anodic electrocatalyst in fields of alkali- and acid-type direct ethanol fuel cells. Copyright © 2016 Elsevier Inc. All rights reserved.

  5. Graphitic Carbon Nitride as a Catalyst Support in Fuel Cells and Electrolyzers

    International Nuclear Information System (INIS)

    Mansor, Noramalina; Miller, Thomas S.; Dedigama, Ishanka; Jorge, Ana Belen; Jia, Jingjing; Brázdová, Veronika; Mattevi, Cecilia; Gibbs, Chris; Hodgson, David; Shearing, Paul R.; Howard, Christopher A.; Corà, Furio; Shaffer, Milo; Brett, Daniel J.L.

    2016-01-01

    Highlights: • Graphitic carbon nitride (gCN) describes many materials with different structures. • gCNs can exhibit excellent mechanical, chemical and thermal resistance. • A major obstacle for pure gCN catalyst supports is limited electronic conductivity. • Composite/Hybrid gCN structures show excellent performance as catalyst supports. • gCNs have great potential for use in fuel calls and water electrolyzers. - Abstract: Electrochemical power sources, such as polymer electrolyte membrane fuel cells (PEMFCs), require the use of precious metal catalysts which are deposited as nanoparticles onto supports in order to minimize their mass loading and therefore cost. State-of-the-art/commercial supports are based on forms of carbon black. However, carbon supports present disadvantages including corrosion in the operating fuel cell environment and loss of catalyst activity. Here we review recent work examining the potential of different varieties of graphitic carbon nitride (gCN) as catalyst supports, highlighting their likely benefits, as well as the challenges associated with their implementation. The performance of gCN and hybrid gCN-carbon materials as PEMFC electrodes is discussed, as well as their potential for use in alkaline systems and water electrolyzers. We illustrate the discussion with examples taken from our own recent studies.

  6. Carbon and Mo transformations during the synthesis of mesoporous Mo2C/carbon catalysts by carbothermal hydrogen reduction

    Science.gov (United States)

    Wang, Haiyan; Liu, Shida; Liu, Bing; Montes, Vicente; Hill, Josephine M.; Smith, Kevin J.

    2018-02-01

    The synthesis of mesoporous Mo2C/carbon catalysts by carbothermal hydrogen reduction is reported. Petroleum coke (petcoke) was activated with KOH at 800 °C to obtain high surface area microporous activated petcoke (APC; 2000 m2/g). The APC was wet impregnated with ammonium heptamolybdate (AHM: 10 wt% Mo), dried and reduced in H2 at temperatures from 400 to 800 °C, to yield Mo2C/APC catalysts. Increased reduction temperature increased the Mo2C yield and the mesoporous volume of the Mo2C/APC. At a reduction temperature of 750 °C the mesopore volume of the catalyst doubled compared to the APC support and accounted for 37% of the total pore volume. Maintaining the final CHR temperature for 90 min further increased the Mo2C yield and mesoporosity of the catalyst. The role of Mo2C in the catalytic hydrogenation of the APC and mesopore generation is demonstrated. The activity of the Mo2C/carbon catalysts in the hydrodeoxygenation of 4-methyl phenol increased with increased CHR temperature and catalyst mesoporosity.

  7. 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.

  8. Cobalt doped CuMnOx catalysts for the preferential oxidation of carbon monoxide

    Science.gov (United States)

    Dey, Subhashish; Dhal, Ganesh Chandra; Mohan, Devendra; Prasad, Ram; Gupta, Rajeev Nayan

    2018-05-01

    Carbon monoxide (CO) is a poisonous gas, recognized as a silent killer for the 21st century. It is produced from the partial oxidation of carbon containing compounds. The catalytic oxidation of CO receives a huge attention due to its applications in different fields. In the present work, hopcalite (CuMnOx) catalysts were synthesized using a co-precipitation method for CO oxidation purposes. Also, it was doped with the cobalt by varying concentration from 1 to 5wt%. It was observed that the addition of cobalt into the CuMnOx catalyst (by the deposition-precipitation method) improved the catalytic performance for the low-temperature CO oxidation. CuMnOx catalyst doped with 3wt% of cobalt exhibited most active performance and showed the highest activity than other cobalt concentrations. Different analytical tools (i.e. XRD, FTIR, BET, XPS and SEM-EDX) were used to characterize the as-synthesized catalysts. It was expected that the introduction of cobalt will introduce new active sites into the CuMnOx catalyst that are associated with the cobalt nano-particles. The order of calcination strategies based on the activity for cobalt doped CuMnOx catalysts was observed as: Reactive calcinations (RC) > flowing air > stagnant air. Therefore, RC (4.5% CO in air) route can be recommended for the synthesis of highly active catalysts. The catalytic activity of doped CuMnOx catalysts toward CO oxidation shows a correlation among average oxidation number of Mn and the position and the nature of the doped cobalt cation.

  9. Preparation of Monodispersed Fe-Mo Nanoparticles as the Catalyst for CVD Synthesis of Carbon Nanotubes

    National Research Council Canada - National Science Library

    Li, Yan; Liu, Jie; Wang, Yongqian; Wang, Zhong L

    2001-01-01

    ...particles were systematically studied. The prepared nanoparticles were used as catalysts for single-walled carbon nanotube growth and the results indicate that there is an upper limit for the size of the catalyst particles to nucleate singlewalled carbon nanotubes.

  10. 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.

  11. Preparation of a Ni-MgO-Al2O3 catalyst with high activity and resistance to potassium poisoning during direct internal reforming of methane in molten carbonate fuel cells

    Science.gov (United States)

    Jang, Won-Jun; Jung, You-Shick; Shim, Jae-Oh; Roh, Hyun-Seog; Yoon, Wang Lai

    2018-02-01

    Steam reforming of methane (SRM) is conducted using a series of Ni-MgO-Al2O3 catalysts for direct internal reforming (DIR) in molten carbonate fuel cells (MCFCs). Ni-MgO-Al2O3 catalysts are prepared by the homogeneous precipitation method with a variety of MgO loading amounts ranging from 3 to 15 wt%. In addition, each precursor concentrations are systemically changed (Ni: 1.2-4.8 mol L-1; Mg: 0.3-1.2 mol L-1; Al: 0.4-1.6 mol L-1) at the optimized composition (10 wt% MgO). The effects of MgO loading and precursor concentration on the catalytic performance and resistance against poisoning of the catalyst by potassium (K) are investigated. The Ni-MgO-Al2O3 catalyst with 10 wt% MgO and the original precursor concentration (Ni: 1.2 mol L-1; Mg: 0.3 mol L-1; Al: 0.4 mol L-1) exhibits the highest CH4 conversion and resistance against K poisoning even at the extremely high gas space velocity (GHSV) of 1,512,000 h-1. Excellent SRM performance of the Ni-MgO-Al2O3 catalyst is attributed to strong metal (Ni) to alumina support interaction (SMSI) when magnesium oxide (MgO) is co-precipitated with the Ni-Al2O3. The enhanced interaction of the Ni with MgO-Al2O3 support is found to protect the active Ni species against K poisoning.

  12. Chelating agent-assisted heat treatment of a carbon-supported iron oxide nanoparticle catalyst for PEMFC.

    Science.gov (United States)

    Liu, Shyh-Jiun; Huang, Chia-Hung; Huang, Chun-Kai; Hwang, Weng-Sing

    2009-08-28

    Iron complexes were supported on commercial carbon black and heat treated to create FeO(x)/C catalysts that showed a larger normalized current density and normalized power density than commercial Pt/C catalysts; the coordination number of the iron complexes used affected the formation of the active site for oxygen reduction in PEMFC.

  13. Dimethyl carbonate synthesis via transesterification of propylene carbonate with methanol by ceria-zinc catalysts: Role of catalyst support and reaction parameters

    Energy Technology Data Exchange (ETDEWEB)

    Kumar, Praveen; Srivastava, Vimal Chandra; Mishra, Indra Mani [Indian Institute of Technology Roorkee, Roorkee 247667, Uttarakhand (India)

    2015-09-15

    Ceria and zinc oxide catalyst were impregnated onto various oxide supports, namely Al{sub 2}O{sub 3}, TiO{sub 2} and SiO{sub 2}, individually by deposition-coprecipitation method. The synthesized catalysts (CZA, CZS and CZT having supports Al{sub 2}O{sub 3}, TiO{sub 2} and SiO{sub 2}, respectively) were characterized by X-ray diffraction (XRD), NH{sub 3}- and CO{sub 2}-temperature programmed desorption (TPD) and N2 adsorption. These catalysts were used for synthesis of dimethyl carbonate (DMC) from methanol and propylene carbonate in a batch reactor. CZS was found to have larger average grain size as compared to CZA and CZT. Composite oxides (catalysts) were found to contain individual phases of ZnO, CeO{sub 2} and some spinel forms of Zn, Ce along with their supports. CZS having highest basicity and surface area showed better catalytic activity as compared to CZA and CZT. Effect of reaction temperature and methanol/PC molar ratio on DMC yield was studied and a reaction mechanism has been discussed. Maximum DMC yield of 77% was observed with CZS catalyst at 170 .deg. C with methanol/PC molar ratio of 10.

  14. Activity and Stability of Nanoscale Oxygen Reduction Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Shao-Horn, Yang

    2015-07-28

    Design of highly active and stable nanoscale catalysts for electro-oxidation of small organic molecules is of great importance to the development of efficient fuel cells. The amount and instability of Pt-based catalysts in the cathode limits the cost, efficiency and lifetime of proton exchange membrane fuel cells. We developed a microscopic understanding of the factors governing activity and stability in Pt and PtM alloys. Experimental efforts were focused on probing the size and shape dependence of ORR activity of Pt-based nanoparticles supported on carbon nanotubes. A microscopic understanding of the activity was achieved by correlating voltammetry and rotating ring disk electrodes to surface atomic and electronic structures, which were elucidated predominantly by high-resolution transmission electron microscopy (HRTEM), Scanning transmission electron microscopy energy dispersive X-ray Spectroscopy (STEM-EDS) and synchrotron X-ray absorption spectroscopy (XAS).

  15. Mechanisms of catalytic activity in heavily coated hydrocracking catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Millan, M.; Adell, C.; Hinojosa, C.; Herod, A.A.; Kandiyoti, R. [University of London Imperial College Science Technology & Medicine, London (United Kingdom). Dept. of Chemical Engineering

    2008-01-15

    Catalyst deactivation by coke deposition has a direct impact on the economic viability of heavy hydrocarbon upgrading processes, such as coal liquefaction and oil residue hydroprocessing. Coke deposition is responsible for rapid loss of catalytic activity and it mostly takes place in the early stages of hydrocracking. The effect of carbonaceous deposition on the catalytic activity of a chromium pillared montmorillonite has been studied in the present work. Its catalytic activity in hydrocracking a coal extract was evaluated based on the boiling point distributions of feed and products obtained by thermogravimetric analysis (TGA), and their characterisation by size exclusion chromatography (SEC) and UV-Fluorescence spectroscopy (UV-F). A large deposition on the catalyst was observed after two successive 2-hour long runs in which the catalyst recovered from the first run was reused in the second. The pillared clay retained its activity even though it showed high carbon loading, a large drop in surface area and complete apparent pore blockage. Some observations may contribute to explain this persistent catalytic activity. First, there is evidence suggesting the dynamic nature of the carbonaceous deposits, which continuously exchange material with the liquid, allowing catalytic activity to continue. Secondly, Scanning Electron Microscopy (SEM) on the used Cr montmorillonite has shown preferential deposition on some regions of the catalyst, which leaves a fraction of the surface relatively exposed. Finally, evidence from SEM coupled to X-ray microanalysis also suggest that deposits are thinner in areas where the active phase of the catalyst is present in higher concentrations. Hydrogenation on the active sites would make the deposits more soluble in the liquid cleaning of surrounding area from deposits.

  16. Pt/glassy carbon model catalysts prepared from PS-b-P2VP micellar templates.

    Science.gov (United States)

    Gu, Yunlong; St-Pierre, Jean; Ploehn, Harry J

    2008-11-04

    Poly(styrene)-block-poly(2-vinylpyridine) (PS-b-P2VP) diblock copolymer was used as a micellar template to fabricate arrays of Pt nanoparticles on mica and glassy carbon (GC) supports. Polymer micellar deposition yields Pt nanoparticles with tunable particle size and surface number density on both mica and GC. After deposition of precursor-loaded micelles onto GC, oxygen plasma etching removes the polymer shell, followed by thermal treatment with H2 gas to reduce the Pt. Etching conditions were optimized to maximize removal of the polymer while minimizing damage to the GC. Arrays of Pt nanoparticles with controlled size and surface number density can be prepared on mica (for particle size characterization) and GC to make Pt/GC model catalysts. These model catalysts were characterized by tapping mode atomic force microscopy, X-ray photoelectron spectroscopy, and cyclic voltammetry to measure activity for oxidation of carbon monoxide or methanol. Cyclic voltammetry results demonstrate the existence of a correlation between Pt particle size and electrocatalytic properties including onset potential, tolerance of carbonaceous adsorbates, and intrinsic activity (based on active Pt area from CO stripping voltammetry). Results obtained with Pt/GC model catalysts duplicate prior results obtained with Pt/porous carbon catalysts therefore validating the synthesis approach and offering a new, tunable platform to study catalyst structure and other effects such as aging on proton exchange membrane fuel cell (PEMFC) reactions.

  17. Electrooxidation of ethanol on novel multi-walled carbon nanotube supported platinum-antimony tin oxide nanoparticle catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Guo, Dao-Jun [School of Chemistry and Chemical Engineering, The Key Laboratory of Life-Organic Analysis, Qufu Normal University, Qufu, Shandong 273165 (China)

    2011-01-15

    We synthesize the new Pt based catalyst for direct ethanol fuel cells using novel multi-walled carbon nanotubes supported platinum-antimony tin oxide (Pt-ATO/MWCNT) nanoparticle as new catalyst support for the first time. The structure of Pt-ATO/MWCNT catalyst is characterized by transmission electron micrograph (TEM) and X-ray diffraction (XRD). The electrocatalytic properties of Pt-ATO/MWCNT catalyst for ethanol electrooxidation reactions are investigated by cyclic voltammetry (CV) and chronoamperometric experiments in acidic medium. The electrocatalytic activity for ethanol electrooxidation reaction shows that high carbon monoxide tolerance and good stability of Pt-ATO/MWCNT catalyst compared with Pt-SnO{sub 2}/MWCNT and commercial Pt/C are observed. These results imply that Pt-ATO/MWCNT catalyst has promising potential applications in direct alcohol fuel cells. (author)

  18. Sea urchin-like mesoporous carbon material grown with carbon nanotubes as a cathode catalyst support for fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Kuo, Ping-Lin; Hsu, Chun-Han; Li, Wan-Ting; Jhan, Jing-Yi; Chen, Wei-Fu [Department of Chemical Engineering, National Cheng Kung University, Tainan 70101 (China)

    2010-12-15

    A sea urchin-like carbon (UC) material with high surface area (416 m{sup 2} g{sup -1}), adequate electrical conductivity (59.6 S cm{sup -1}) and good chemical stability was prepared by growing carbon nanotubes onto mesoporous carbon hollow spheres. A uniform dispersion of Pt nanoparticles was then anchored on the UC, where the Pt nanoparticles were prepared using benzylamine as the stabilizer. For this Pt loaded carbon, cyclic voltammogram measurements showed an exceptionally high electrochemically active surface area (EAS) (114.8 m{sup 2} g{sup -1}) compared to the commonly used commercial E-TEK catalyst (65.2 m{sup 2} g{sup -1}). The durability test demonstrates that the carbon used as a support exhibited minor loss in EAS of Pt. Compared to the E-TEK (20 wt%) cathode catalyst, this Pt loaded UC catalyst has greatly enhanced catalytic activity toward the oxygen reduction reaction, less cathode flooding and considerably improved performance, resulting in an enhancement of ca. 37% in power density compared with that of E-TEK. Based on the results obtained, the UC is an excellent support for Pt nanoparticles used as cathode catalysts in proton exchange membrane fuel cells. (author)

  19. A Study of Iron-Nitrogen-Carbon Fuel Cell Catalysts: Chemistry - Nanostructure - Performance

    Science.gov (United States)

    Workman, Michael J., Jr.

    focused ion beam tomography is modified and optimized for platinum-group metal free catalyst layers, facilitating direct observation of catalyst integration into catalyst layers. I present evidence supporting the hypothesis that atomically dispersed iron coordinated with nitrogen are the dominant active sites in these catalysts. Further, that the concentration of surface oxides in the carbon structure, which can be directly influenced by synthesis parameters, correlates with both the concentration of active sites in the material and with fuel cell performance. Catalyst performance is hindered by the addition of carbon nanotubes and by the presence of metallic iron. Evidence consistent with the catalytic active sites residing in the graphitic plane is also presented.

  20. 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

  1. A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels.

    Science.gov (United States)

    Qiao, Jinli; Liu, Yuyu; Hong, Feng; Zhang, Jiujun

    2014-01-21

    This paper reviews recent progress made in identifying electrocatalysts for carbon dioxide (CO2) reduction to produce low-carbon fuels, including CO, HCOOH/HCOO(-), CH2O, CH4, H2C2O4/HC2O4(-), C2H4, CH3OH, CH3CH2OH and others. The electrocatalysts are classified into several categories, including metals, metal alloys, metal oxides, metal complexes, polymers/clusters, enzymes and organic molecules. The catalyts' activity, product selectivity, Faradaic efficiency, catalytic stability and reduction mechanisms during CO2 electroreduction have received detailed treatment. In particular, we review the effects of electrode potential, solution-electrolyte type and composition, temperature, pressure, and other conditions on these catalyst properties. The challenges in achieving highly active and stable CO2 reduction electrocatalysts are analyzed, and several research directions for practical applications are proposed, with the aim of mitigating performance degradation, overcoming additional challenges, and facilitating research and development in this area.

  2. Catalytic Growth of Macroscopic Carbon Nanofibers Bodies with Activated Carbon

    Science.gov (United States)

    Abdullah, N.; Rinaldi, A.; Muhammad, I. S.; Hamid, S. B. Abd.; Su, D. S.; Schlogl, R.

    2009-06-01

    Carbon-carbon composite of activated carbon and carbon nanofibers have been synthesized by growing Carbon nanofiber (CNF) on Palm shell-based Activated carbon (AC) with Ni catalyst. The composites are in an agglomerated shape due to the entanglement of the defective CNF between the AC particles forming a macroscopic body. The macroscopic size will allow the composite to be used as a stabile catalyst support and liquid adsorbent. The preparation of CNT/AC nanocarbon was initiated by pre-treating the activated carbon with nitric acid, followed by impregnation of 1 wt% loading of nickel (II) nitrate solutions in acetone. The catalyst precursor was calcined and reduced at 300° C for an hour in each step. The catalytic growth of nanocarbon in C2H4/H2 was carried out at temperature of 550° C for 2 hrs with different rotating angle in the fluidization system. SEM and N2 isotherms show the level of agglomeration which is a function of growth density and fluidization of the system. The effect of fluidization by rotating the reactor during growth with different speed give a significant impact on the agglomeration of the final CNF/AC composite and thus the amount of CNFs produced. The macrostructure body produced in this work of CNF/AC composite will have advantages in the adsorbent and catalyst support application, due to the mechanical and chemical properties of the material.

  3. Valorization of waste Date pits biomass for biodiesel production in presence of green carbon catalyst

    International Nuclear Information System (INIS)

    Abu-Jrai, Ahmad M.; Jamil, Farrukh; Al-Muhtaseb, Ala'a H.; Baawain, Mahad; Al-Haj, Lamya; Al-Hinai, Mohab; Al-Abri, Mohammed; Rafiq, Sikander

    2017-01-01

    Highlights: • Waste Date pits were utilized to produce green catalyst for biodiesel production. • The optimized yield of biodiesel was 91.6% at 65 °C and 9:1 methanol to oil ratio. • Catalyst activity decreases very less upon reusing it up to three runs. • Produced biodiesel possess competent fuel properties as per ASTM and EN standards. - Abstract: In this study, an efficient utilization of waste Date pits biomass for synthesizing green carbon catalyst as well as production of biodiesel were investigated. The green carbon catalyst was modified by KOH and characterized by XRD, SEM, EDX, TEM and BET. Taguchi method in Response Surface Methodology (RSM) was applied to study the effect of several process parameters such as reaction temperature, time, catalysts type and methanol to oil ratio, on the yield of the produced biodiesel. The optimized yield obtained was 91.6% when the process temperature was 65 °C, with catalyst type C3 (6 wt% KOH on carbon) within 1 h and with 9:1 methanol to oil ratio. The produced biodiesel was completely characterized in order to verify its quality, compared with the international standards. Fuel properties of the produced biodiesel were found to be a cetane number 60.31, density 881 kg/m"3, viscosity 4.24 mm"2/s, cloud point 3.9 °C, cold filter plugging point −0.62 °C, pour point −1.4 °C and flash point 141 °C, which lies within the limits specified by the international standards of ASTM and EN. Waste Date pits biomass can be a promising platform for the production of green carbon catalysts as well as biodiesel production.

  4. Efficient selective catalytic reduction of NO by novel carbon-doped metal catalysts made from electroplating sludge.

    Science.gov (United States)

    Zhang, Jia; Zhang, Jingyi; Xu, Yunfeng; Su, Huimin; Li, Xiaoman; Zhou, Ji Zhi; Qian, Guangren; Li, Li; Xu, Zhi Ping

    2014-10-07

    Electroplating sludges, once regarded as industrial wastes, are precious resources of various transition metals. This research has thus investigated the recycling of an electroplating sludge as a novel carbon-doped metal (Fe, Ni, Mg, Cu, and Zn) catalyst, which was different from a traditional carbon-supported metal catalyst, for effective NO selective catalytic reduction (SCR). This catalyst removed >99.7% NO at a temperature as low as 300 °C. It also removed NO steadily (>99%) with a maximum specific accumulative reduced amount (MSARA) of 3.4 mmol/g. Gas species analyses showed that NO removal was accompanied by evolving N2 and CO2. Moreover, in a wide temperature window, the sludge catalyst showed a higher CO2 selectivity (>99%) than an activated carbon-supported metal catalyst. Structure characterizations revealed that carbon-doped metal was transformed to metal oxide in the sludge catalyst after the catalytic test, with most carbon (2.33 wt %) being consumed. These observations suggest that NO removal over the sludge catalyst is a typical SCR where metals/metal oxides act as the catalytic center and carbon as the reducing reagent. Therefore, our report probably provides an opportunity for high value-added utilizations of heavy-metal wastes in mitigating atmospheric pollutions.

  5. Dehydrogenation of Ethylbenzene with Carbon Dioxide as Soft Oxidant over Supported Vanadium-Antimony Oxide Catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Hong, Do Young; Vislovskiy, Vladislav P.; Yoo, Jin S.; Chang, Jong San [Korea Research Institute of Chemical Technology, Daejeon (Korea, Republic of); Park, Sang Eon [Inha University, Incheon (Korea, Republic of); Park, Min Seok [Mongolia International University, Ulaanbaatar (Mongolia)

    2005-11-15

    This work presents that carbon dioxide, which is a main contributor to the global warming effect, could be utilized as a selective oxidant in the oxidative dehydrogenation of ethylbenzene. The dehydrogenation of ethylbenzene over alumina-supported vanadium-antimony oxide catalyst has been studied under different atmospheres such as inert nitrogen, steam, oxygen or carbon dioxide as diluent or oxidant. Among them, the addition of carbon dioxide gave the highest styrene yield (up to 82%) and styrene selectivity (up to 97%) along with stable activity. Carbon dioxide could play a beneficial role of a selective oxidant in the improvement of the catalytic behavior through the oxidative pathway.

  6. Control of carbon nanotube growth using cobalt nanoparticles as catalyst

    International Nuclear Information System (INIS)

    Huh, Yoon; Green, Malcolm L.H.; Kim, Young Heon; Lee, Jeong Yong; Lee, Cheol Jin

    2005-01-01

    We have controllably grown carbon nanotubes using uniformly distributed cobalt nanoparticles as catalyst. Cobalt nanoparticles with a uniform size were synthesized by chemical reaction and colloidal solutions including the cobalt nanoparticles were prepared. The cobalt nanoparticles were uniformly distributed on silicon substrates by a spin-coating method. Carbon nanotubes with a uniform diameter were synthesized on the cobalt nanoparticles by thermal chemical vapor deposition of acetylene gas. The density and vertical alignment of carbon nanotubes could be controlled by adjusting the density of cobalt (Co) nanoparticles

  7. The Mossbauer spectra of carbon nanotubes synthesize using ferrite catalyst

    International Nuclear Information System (INIS)

    Zhang Haiyan; Lin Jiapeng; Peng Zuxiong; Zeng Guoxun; Pang Jinshan; Chen Yiming

    2009-01-01

    The ferrite powder with honeycombed structure obtained by chemical combustion was used as catalyst to synthesize multi-walled carbon nanotubes by chemical vapor deposition. The magnetic components and characters of the the carbon nanotubes synthesized were investigated by X-ray diffraction (XRD), Mossbauer spectra and vibrating-sample magnetometer (VSM). The ferric components of the carbon nanotubes samples can be identified by Mossbauer spectra. The Mossbauer spectra of carbon nanotubes sample after purification contains two ferromagnetic sextet components corresponding to α-Fe species and Fe 3 C (cementite) species. While the Mossbauer spectra of the carbon nanotubes sample before purification contains three ferromagnetic sextet components corresponding to α-Fe species, Fe 3 C species and γ-Fe 2 O 3 . The saturation magnetization intensity Ms of carbon nanotubes sample after purification is decreased from 46.61 to 2.94 emu/g, but the coercive force increasd and reached 328Oe.

  8. Hydrogen production by dry reforming of methane with carbon dioxide in one-dimensional nickel-based catalysts

    International Nuclear Information System (INIS)

    Lopez U, A. C.

    2016-01-01

    The main objective of this thesis is development of nickel catalysts supported over 1D matrix of cerium oxide, to be used in dry reforming methane reaction with carbon dioxide for hydrogen production. The catalysts were characterized by: Temperature Programmed Reduction (TPR), Scanning Electronic Microscopy (Sem), Surface Area (Bet method) an X Ray Diffraction (XRD). The TPR technique allowed to define reduction temperature of the active phase in the catalyst, Sem technique showed that the CeO_2 matrix had a nano rod morphology. XRD allowed to identify the crystalline phases of the catalysts. Finally, the catalysts were tested in the dry reforming methane reaction, high catalytic activity and hydrogen production were performed at 700 degrees Celsius and the catalyst with 30 wt.% of nickel. (Author)

  9. Turbostratic carbon supported palladium as an efficient catalyst for reductive purification of water from trichloroethylene

    Directory of Open Access Journals (Sweden)

    Emil Kowalewski

    2017-12-01

    Full Text Available This work investigates the catalytic properties of turbostratic carbon supported Pd catalyst in hydrodechlorination of trichloroethylene (TCE HDC in aqueous phase. 1.57 wt% Pd/C was thoroughly characterized by BET, TPHD, CO chemisorption, PXRD, STEM, XPS and used as the catalyst in removal of trichloroethylene from drinking water in batch and continuous-flow reactors. The studies showed that catalytic performance of Pd/C depended on the hydrophobicity and textural properties of carbon support, which influenced noble metal dispersion and increased catalyst tolerance against deactivation by chlorination. Palladium in the form of uniformly dispersed small (~3.5 nm nanoparticles was found to be very active and stable in purification of water from TCE both in batch and continuous-flow operation.

  10. 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.

  11. The kinetics of steam-carbon dioxide conversion, rational ways and production catalysts of process gas

    International Nuclear Information System (INIS)

    Khamroev, F.B.

    2016-01-01

    The purpose of the present work is to study the kinetics of steam-carbon dioxide conversion, rational ways and production catalysts of process gas. The experimental equation of steam-carbon methane conversion, heat stability increasing and catalyst efficiency, decreasing of hydrodynamical resistance of catalyst layer were determined.

  12. Carbon-supported cubic CoSe2 catalysts for oxygen reduction reaction in alkaline medium

    International Nuclear Information System (INIS)

    Feng Yongjun; Alonso-Vante, Nicolas

    2012-01-01

    Highlights: ► Cubic CoSe 2 a non-precious metal electrocatalyst for oxygen reduction in KOH. ► The catalyst shows four-electron transfer pathway in overall reaction. ► Catalyst has higher methanol tolerance than commercial Pt/C catalyst. - Abstract: A Carbon-supported CoSe 2 nanocatalyst has been developed as an alternative non-precious metal electrocatalyst for oxygen reduction reaction (ORR) in alkaline medium. The catalyst was prepared via a surfactant-free route and its electrocatalytic activity for the ORR has been investigated in detail in 0.1 M KOH electrolyte at 25 °C using rotating disk electrode (RDE) and rotating ring-disk electrode (RRDE) techniques. The prepared catalyst showed promising catalytic activity towards ORR in a four-electron transfer pathway and higher tolerance to methanol compared to commercial Pt/C catalyst in 0.1 M KOH. To some extent, the increase of CoSe 2 loading on the electrode favors a faster reduction of H 2 O 2 intermediate to H 2 O.

  13. Process of activation of a palladium catalyst system

    Science.gov (United States)

    Sobolevskiy, Anatoly [Orlando, FL; Rossin, Joseph A [Columbus, OH; Knapke, Michael J [Columbus, OH

    2011-08-02

    Improved processes for activating a catalyst system used for the reduction of nitrogen oxides are provided. In one embodiment, the catalyst system is activated by passing an activation gas stream having an amount of each of oxygen, water vapor, nitrogen oxides, and hydrogen over the catalyst system and increasing a temperature of the catalyst system to a temperature of at least 180.degree. C. at a heating rate of from 1-20.degree./min. Use of activation processes described herein leads to a catalyst system with superior NOx reduction capabilities.

  14. Magnetism for understanding catalyst analysis of purified carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Bellouard, Christine; Mercier, Guillaume; Cahen, Sébastien; Ghanbaja, Jaafar; Medjahdi, Ghouti [Institut Jean Lamour, CNRS-Université de Lorraine, BP 70239, 54506 Vandoeuvre-lès-Nancy (France); Gleize, Jérôme [Laboratoire de Chimie Physique-Approche Multi-échelle de Milieux Complexes-Université de Lorraine, 1 Bd Arago, 57078 Metz (France); Lamura, Gianrico [CNR-SPIN – Dipartimento di Fisica, via Dodecaneso 33, 16146 Genova (Italy); Hérold, Claire [Institut Jean Lamour, CNRS-Université de Lorraine, BP 70239, 54506 Vandoeuvre-lès-Nancy (France); Vigolo, Brigitte, E-mail: Brigitte.Vigolo@univ-lorraine.fr [Institut Jean Lamour, CNRS-Université de Lorraine, BP 70239, 54506 Vandoeuvre-lès-Nancy (France)

    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 Ni{sup 2+} ions, belonging to NiCl{sub 2} formed during the Cl-based purification process. In particular, NiCl{sub 2} 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. - Highlights: • Cl-gas treatment of Ni catalyst of carbon nanotubes leads to NiCl{sub 2} residue. • Magnetic measurements show the transformation of Ni{sup 0} in Ni{sup 2+}through a purification process. • High temperature Cl treatment removes 75% of metallic impurities. • Cl-purification yields to an amount of metal of 1.5% in arc-discharge CNT samples.

  15. Steam dealkylation catalyst and a method for its activation

    International Nuclear Information System (INIS)

    Dorawala, T.; Reinhard, R.

    1980-01-01

    The method of activating a supported catalyst containing oxides of a group viii metal and of a group 1 a metal which comprises heating said catalyst at a rate of 10 0 to 500 0 F/hr to a temperature of 650 0 to 1400 0 F in a hydrogen atmosphere; maintaining said heated catalyst in a hydrogen atmosphere at 650 0 to 1400 0 F for 2 to 30 hours thereby forming a hydrogen-treated catalyst; and maintaining the hydrogen-treated catalyst in a steam-hydrogen atmosphere at 650 0 to 1400 0 F for 2 to 20 hours thereby forming a steamed hydrogen-treated catalyst

  16. Synthesis of Dimethyl Glutarate from Cyclobutanone and Dimethyl Carbonate over Solid Base Catalysts

    International Nuclear Information System (INIS)

    Zhi, Chen; Dudu, Wu

    2012-01-01

    A facile route for the synthesis of dimethyl glutarate (DMG) from cyclobutanone and dimethyl carbonate (DMC) in the presence of solid base catalysts has been developed. It was found that the intermediate carbomethoxycyclobutanone (CMCB) was produced from cyclobutanone with DMC in the first step, and then CMCB was further converted to DMG by reacting with a methoxide group. The role of the basic catalysts can be mainly ascribed to the activation of cyclobutanone via the abstraction of a proton in the α-position by base sites, and solid bases with moderate strength, such as MgO, favor the formation of DMG

  17. Synthesis of Dimethyl Glutarate from Cyclobutanone and Dimethyl Carbonate over Solid Base Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Zhi, Chen; Dudu, Wu [Guangdong Medical College, Dongguan (China)

    2012-06-15

    A facile route for the synthesis of dimethyl glutarate (DMG) from cyclobutanone and dimethyl carbonate (DMC) in the presence of solid base catalysts has been developed. It was found that the intermediate carbomethoxycyclobutanone (CMCB) was produced from cyclobutanone with DMC in the first step, and then CMCB was further converted to DMG by reacting with a methoxide group. The role of the basic catalysts can be mainly ascribed to the activation of cyclobutanone via the abstraction of a proton in the {alpha}-position by base sites, and solid bases with moderate strength, such as MgO, favor the formation of DMG

  18. Effect of the dispersants on Pd species and catalytic activity of supported palladium catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Yue [Key Laboratory for Green Chemical Process of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205 (China); Yang, Xiaojun, E-mail: 10100201@wit.edu.cn [Key Laboratory for Green Chemical Process of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205 (China); Cao, Shuo, E-mail: cao23@email.sc.edu [North America R& D Center, Clariant BU Catalysts, Louisville, 40209, KY (United States); Zhou, Jie [Key Laboratory for Green Chemical Process of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205 (China); Wu, Yuanxin [Key Laboratory for Green Chemical Process of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205 (China); School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China); Han, Jinyu [School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China); Yan, Zhiguo [Key Laboratory for Green Chemical Process of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205 (China); Zheng, Mingming [Oil Crops Research Institute, Chinese Academy of Agricultural Sciences, Hubei Key Laboratory of Oilcrops Lipid Chemistry and Nutrition, Wuhan 430062 (China)

    2017-04-01

    Highlights: • Polyvinyl alcohol (PVA) inhibited the sintering and reduction of Pd nanoparticles. • Activity was improved for supported Pd catalysts with PVA modified method. • PVA modified method minimized the catalyst deactivation. • This work provides an insight of the regeneration strategies for Pd catalysts. - Abstract: A series of supported palladium catalysts has been prepared through the precipitation method and the reduction method, using polyvinyl alcohol (PVA) and polyvinylpyrrolidone (PVP) as dispersants. The effects of the dispersants on the properties of catalysts were evaluated and the catalytic performance of the new materials was investigated for the oxidative carbonylation of phenol to diphenyl carbonate (DPC). The catalysts as prepared were also characterized by the X-ray diffraction (XRD), transmission electron microscope (TEM), Brunner-Emmet-Teller (BET) measurements and X-ray photoelectron spectroscopy (XPS) techniques. The results show that the addition of the dispersants had no effect on the crystal phase of the catalysts. However, the dispersion of Pd particles was improved when the dispersants were used. Moreover, the particle sizes of Pd nanoparticles modified by PVA were smaller than those modified by PVP. The catalysts prepared using the dispersants gave better yields of DPC than the catalysts prepared without the dispersants. The highest yield of DPC was 17.9% with the PVA-Red catalyst. The characterization results for the used catalysts showed that the Pd species in the PVA-Red catalyst remained mostly divalent and the lattice oxygen species were consumed during the reaction, which could lead to the higher catalytic activity of the PVA-Red catalyst. The experimental results confirm that PVA effectively inhibited the sintering and reduction of active Pd species in the oxidative carbonylation of phenol.

  19. Fe catalysts for methane decomposition to produce hydrogen and carbon nano materials

    KAUST Repository

    Zhou, Lu; Enakonda, Linga Reddy; Harb, Moussab; Saih, Youssef; Aguilar Tapia, Antonio; Ould-Chikh, Samy; Hazemann, Jean-louis; Li, Jun; Wei, Nini; Gary, Daniel; Del-Gallo, Pascal; Basset, Jean-Marie

    2017-01-01

    Conducting catalytic methane decomposition over Fe catalysts is a green and economic route to produce H2 without CO/CO2 contamination. Fused 65wt% and impregnated 20wt% Fe catalysts were synthesized with different additives to investigate their activity, whereas showing Fe-Al2O3 combination as the best catalyst. Al2O3 is speculated to expose more Fe00 for the selective deposition of carbon nano tubes (CNTs). A fused Fe (65wt%)-Al2O3 sample was further investigated by means of H2-TPR, in-situ XRD, HRTEM and XAS to conclude 750°C is the optimized temperature for H2 pre-reduction and reaction to obtain a high activity. Based on density functional theory (DFT) study, a reaction mechanism over Fe catalysts was proposed to explain the formation of graphite from unstable supersaturated iron carbides decomposition. A carbon deposition model was further proposed which explains the formation of different carbon nano materials.

  20. Fe catalysts for methane decomposition to produce hydrogen and carbon nano materials

    KAUST Repository

    Zhou, Lu

    2017-02-21

    Conducting catalytic methane decomposition over Fe catalysts is a green and economic route to produce H2 without CO/CO2 contamination. Fused 65wt% and impregnated 20wt% Fe catalysts were synthesized with different additives to investigate their activity, whereas showing Fe-Al2O3 combination as the best catalyst. Al2O3 is speculated to expose more Fe00 for the selective deposition of carbon nano tubes (CNTs). A fused Fe (65wt%)-Al2O3 sample was further investigated by means of H2-TPR, in-situ XRD, HRTEM and XAS to conclude 750°C is the optimized temperature for H2 pre-reduction and reaction to obtain a high activity. Based on density functional theory (DFT) study, a reaction mechanism over Fe catalysts was proposed to explain the formation of graphite from unstable supersaturated iron carbides decomposition. A carbon deposition model was further proposed which explains the formation of different carbon nano materials.

  1. High utilization platinum deposition on single-walled carbon nanotubes as catalysts for direct methanol fuel cell

    International Nuclear Information System (INIS)

    Wang, J.J.; Yin, G.P.; Zhang, J.; Wang, Z.B.; Gao, Y.Z.

    2007-01-01

    This research aims to enhance the activity of Pt catalysts, thus to lower the loading of Pt metal in fuel cell. Highly dispersed platinum supported on single-walled carbon nanotubes (SWNTs) as catalyst was prepared by ion exchange method. The homemade Pt/SWNTs underwent a repetition of ion exchange and reduction process in order to achieve an increase of the metal loading. For comparison, the similar loading of Pt catalyst supported on carbon nanotubes was prepared by borohydride reduction method. The catalysts were characterized by using energy dispersive analysis of X-ray (EDAX), transmission electron micrograph (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectrum (XPS). Compared with the Pt/SWNTs catalyst prepared by borohydride method, higher Pt utilization was achieved on the SWNTs by ion exchange method. Furthermore, in comparison to the E-TEK 20 wt.% Pt/C catalyst with the support of carbon black, the results from electrochemical measurement indicated that the Pt/SWNTs prepared by ion exchange method displayed a higher catalytic activity for methanol oxidation and higher Pt utilization, while no significant increasing in the catalytic activity of the Pt/SWNTs catalyst obtained by borohydride method

  2. Controllable pt nanoparticle deposition on carbon nanotubes as an anode catalyst for direct methanol fuel cells.

    Science.gov (United States)

    Mu, Yongyan; Liang, Hanpu; Hu, Jinsong; Jiang, Li; Wan, Lijun

    2005-12-01

    We report a novel process to prepare well-dispersed Pt nanoparticles on CNTs. Pt nanoparticles, which were modified by the organic molecule triphenylphosphine, were deposited on multiwalled carbon nanotubes by the organic molecule, which acts as a cross linker. By manipulating the relative ratio of Pt nanoparticles and multiwalled carbon nanotubes in solution, Pt/CNT composites with different Pt content were achieved. The so-prepared Pt/CNT composite materials show higher electrocatalytic activity and better tolerance to poisoning species in methanol oxidation than the commercial E-TEK catalyst, which can be ascribed to the high dispersion of Pt nanoparticles on the multiwalled carbon nanotube surface.

  3. Hydrodeoxygenation of phenols as lignin models under acid-free conditions with carbon-supported platinum catalysts.

    Science.gov (United States)

    Ohta, Hidetoshi; Kobayashi, Hirokazu; Hara, Kenji; Fukuoka, Atsushi

    2011-11-28

    Carbon-supported Pt catalysts are highly active and reusable for the aqueous-phase hydrodeoxygenation of phenols as lignin models without adding any acids. It is suggested that Pt/carbon facilitates the hydrogenation of phenols and the hydrogenolysis of the resulting cyclohexanols.

  4. A Simple Synthesis of an N-Doped Carbon ORR Catalyst: Hierarchical Micro/Meso/Macro Porosity and Graphitic Shells

    NARCIS (Netherlands)

    Eisenberg, D.; Stroek, W.; Geels, N.J.; Sandu, C.S.; Heller, A.; Yan, N.; Rothenberg, G.

    2016-01-01

    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

  5. Heterogeneous electrochemical CO2 reduction using nonmetallic carbon-based catalysts: current status and future challenges

    Science.gov (United States)

    Ma, Tao; Fan, Qun; Tao, Hengcong; Han, Zishan; Jia, Mingwen; Gao, Yunnan; Ma, Wangjing; Sun, Zhenyu

    2017-11-01

    Electrochemical CO2 reduction (ECR) offers an important pathway for renewable energy storage and fuels production. It still remains a challenge in designing highly selective, energy-efficient, robust, and cost-effective electrocatalysts to facilitate this kinetically slow process. Metal-free carbon-based materials have features of low cost, good electrical conductivity, renewability, diverse structure, and tunability in surface chemistry. In particular, surface functionalization of carbon materials, for example by doping with heteroatoms, enables access to unique active site architectures for CO2 adsorption and activation, leading to interesting catalytic performances in ECR. We aim to provide a comprehensive review of this category of metal-free catalysts for ECR, providing discussions and/or comparisons among different nonmetallic catalysts, and also possible origin of catalytic activity. Fundamentals and some future challenges are also described.

  6. Carbon nanotubes and other nanostructures as support material for nanoparticulate noble-metal catalysts in fuel cells

    DEFF Research Database (Denmark)

    Veltzé, Sune; Larsen, Mikkel Juul; Elina, Yli-Rantala

    or platinum-alloy catalysts in the electrodes are required. To maximize the utilization of the noble metal it is frequently deposited as nanoparticles (1–5 nm) on a stabilizing support of carbon black. Carbon black provides good anchoring of the catalyst particles, but is prone to severe destructive oxidation...... at high electrical potentials encountered occasionally in fuel cells. Other nanostructures of carbon are being investigated as alternatives to carbon black as they have several beneficial properties. Multi-walled carbon nanotubes (MW-CNT) are an example of one type of these promising materials. Like...... of the fuel-cell electrodes. However, the low concentration of structural defects also poses challenges with regard to anchoring of the catalyst particles on the CNT surface. Thus, activation treatments introducing surface functional groups may be necessary. Also, the surface properties are responsible...

  7. Facile preparation of hierarchically porous carbon using diatomite as both template and catalyst and methylene blue adsorption of carbon products.

    Science.gov (United States)

    Liu, Dong; Yuan, Peng; Tan, Daoyong; Liu, Hongmei; Wang, Tong; Fan, Mingde; Zhu, Jianxi; He, Hongping

    2012-12-15

    Hierarchically porous carbons were prepared using a facile preparation method in which diatomite was utilized as both template and catalyst. The porous structures of the carbon products and their formation mechanisms were investigated. The macroporosity and microporosity of the diatomite-templated carbons were derived from replication of diatom shell and structure-reconfiguration of the carbon film, respectively. The macroporosity of carbons was strongly dependent on the original morphology of the diatomite template. The macroporous structure composed of carbon plates connected by the pillar- and tube-like macropores resulted from the replication of the central and edge pores of the diatom shells with disk-shaped morphology, respectively. And another macroporous carbon tubes were also replicated from canoe-shaped diatom shells. The acidity of diatomite dramatically affected the porosity of the carbons, more acid sites of diatomite template resulted in higher surface area and pore volume of the carbon products. The diatomite-templated carbons exhibited higher adsorption capacity for methylene blue than the commercial activated carbon (CAC), although the specific surface area was much smaller than that of CAC, due to the hierarchical porosity of diatomite-templated carbons. And the carbons were readily reclaimed and regenerated. Copyright © 2012 Elsevier Inc. All rights reserved.

  8. Upgrading of glycerol from biodiesel synthesis with dimethyl carbonate on reusable Sr–Al mixed oxide catalysts

    International Nuclear Information System (INIS)

    Algoufi, Y.T.; Akpan, U.G.; Kabir, G.; Asif, M.; Hameed, B.H.

    2017-01-01

    Highlights: • Catalytic transesterification with dimethyl carbonate (DMC) converts glycerol into glycerol carbonate (GLC). • DMC and Sr_x–Al catalysts affect the reaction mechanisms that convert glycerol into GLC. • The morphology and textural structure of Sr_x–Al catalysts perpetuate catalytic activity. • The atomic ratio of Sr/Al has a unique effect on Sr–Al catalytic activity. • Sr_0_._5–Al catalyst exhibits limited leaching after five reaction cycles. - Abstract: The high demand for renewable energy has led to the upsurge of methanol-assisted biodiesel synthesis. Therefore, glycerol as a byproduct entered the waste stream given the oversupply of biodiesel to the market. The dimethyl carbonate (DMC)-assisted transesterification of glycerol on a catalyst has been a popular approach for converting glycerol into valuable glycerol carbonate (GLC). The synthesis of GLC from the DMC-assisted transesterification of glycerol on mixed oxide catalysts (Sr_x–Al) with different Sr/Al ratios was examined in this study. A glycerol conversion of 99.4% and a GLC yield of 100% were achieved in a catalyst with Sr/Al = 0.5 (Sr_0_._5–Al). Both values are higher than those in catalysts synthesized with Sr/Al = 0.25 and 0.75. The Sr_0_._5–Al catalyst withstood five transesterification reaction cycles without a serious deactivation induced by the leaching of active SrO. Therefore, the Sr_0_._5–Al catalyst is suitable for consecutive uses in the DMC-assisted transesterification of glycerol with DMC into GLC.

  9. Development of Sulfur and Carbon Tolerant Reforming Alloy Catalysts Aided Fundamental Atomistic Insights

    Energy Technology Data Exchange (ETDEWEB)

    Suljo Linic

    2008-12-31

    Current hydrocarbon reforming catalysts suffer from rapid carbon and sulfur poisoning. Even though there is a tremendous incentive to develop more efficient catalysts, these materials are currently formulated using inefficient trial and error experimental approaches. We have utilized a hybrid experimental/theoretical approach, combining quantum Density Functional Theory (DFT) calculations and various state-of-the-art experimental tools, to formulate carbon tolerant reforming catalysts. We have employed DFT calculations to develop molecular insights into the elementary chemical transformations that lead to carbon poisoning of Ni catalysts. Based on the obtained molecular insights, we have identified, using DFT quantum calculation, various Ni alloy catalysts as potential carbon tolerant reforming catalysts. The alloy catalysts were synthesized and tested in steam reforming and partial oxidation of methane, propane, and isooctane. We demonstrated that the alloy catalysts are much more carbon-tolerant than monometallic Ni catalysts under nearly stoichiometric steam-to-carbon ratios. Under these conditions, monometallic Ni is rapidly poisoned by sp2 carbon deposits. The research approach is distinguished by two characteristics: (a) knowledge-based, bottomup approach, compared to the traditional trial and error approach, allows for a more efficient and systematic discovery of improved catalysts. (b) the focus is on exploring alloy materials which have been largely unexplored as potential reforming catalysts.

  10. Performance of (CoPC)n catalyst in active lithium-thionyl chloride cells

    Science.gov (United States)

    Shah, Pinakin M.

    1990-01-01

    An experimental study was conducted with anode limited D size cells to characterize the performance of an active lithium-thionyl chloride (Li/SOCl2) system using the polymeric cobalt phthalocyanine, (CoPC)n, catalyst in carbon cathodes. The author describes the results of this experiment with respect to initial voltage delays, operating voltages, and capacities. The effectiveness of the preconditioning methods evolved to alleviate passivation effects on storage are also discussed. The results clearly demonstrated the superior high rate capability of cells with the catalyst. The catalyst did not adversely impact the performance of cells after active storage for up to 6 months, while retaining its beneficial influences.

  11. Promotional effect of phosphorus doping on the activity of the Fe-N/C catalyst for the oxygen reduction reaction

    DEFF Research Database (Denmark)

    Hu, Yang; Zhu, Jianbin; Lv, Qing

    2015-01-01

    Cost-effective, active and stable electrocatalysts for the oxygen reduction reaction (ORR) are highly desirable for the wide-spread adoption of technologies such as fuel cells and metal-air batteries. Among the already reported non-precious metal catalysts, carbon-supported transition metal...... to that for the undoped Fe-N/C catalyst. The activity and durability of the catalysts are demonstrated in direct methanol fuel cells....

  12. Carbon-supported iron and iron-molybdenum sulfide catalysts

    International Nuclear Information System (INIS)

    Ramselaar, W.L.T.M.

    1988-01-01

    The main objective was to describe the relations between the characteristics (composition and dispersion) of the actual sulfide phase and the catalytic activity. Attention was also paid to the influence of preparational aspects on these characteristics. The catalysts were characterized using in-situ Moessbauer spectroscopy down to 2.0 K. 254 refs.; 47 figs.; 22 tabs

  13. Cationic Zn-Porphyrin Polymer Coated onto CNTs as a Cooperative Catalyst for the Synthesis of Cyclic Carbonates.

    Science.gov (United States)

    Jayakumar, Sanjeevi; Li, He; Chen, Jian; Yang, Qihua

    2018-01-24

    The development of solid catalysts containing multiple active sites that work cooperatively is very attractive for biomimetic catalysis. Herein, we report the synthesis of bifunctional catalysts by supporting cationic porphyrin-based polymers on carbon nanotubes (CNTs) using the direct reaction of 5,10,15,20-tetrakis(4-pyridyl)porphyrin zinc(II), di(1H-imidazol-1-yl)methane, and 1,4-bis(bromomethyl)benzene in the presence of CNTs. The bifunctional catalysts could efficiently catalyze the cycloaddition reaction of epoxides and CO 2 under solvent-free conditions with porphyrin zinc(II) as the Lewis acid site and a bromine anion as a nucleophilic agent working in a cooperative way. Furthermore, a relative amount of porphyrin zinc(II) and quaternary ammonium bromide could be facilely adjusted for facilitating cooperative behavior. The bifunctional catalyst with a TOF up to 2602 h -1 is much more active than the corresponding homogeneous counterpart and is one of the most active heterogeneous catalysts ever reported under cocatalyst-free conditions. The high activity is mainly attributed to the enhanced cooperation effect of the bifunctional catalyst. With a wide substrate scope, the bifunctional catalyst could be stably recycled. This work demonstrates a new approach for the generation of a cooperative activation effect for solid catalysts.

  14. 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.

  15. Promoting effect of active carbons on methanol dehydrogenation on sodium carbonate - hydrogen spillover

    OpenAIRE

    Su, S.; Prairie, M.; Renken, A.

    1993-01-01

    Methanol dehydrogenation to formaldehyde was conducted in a fixed-bed flow reactor with sodium carbonate catalyst mixed with active carbons or transition metals. The additives promoted the reaction rate at 880-970 K without modifying formaldehyde selectivity. This effect increases with increasing carbon content in the carbon-carbonate mixture. Activation energy of methanol conversion is the same for the mixture and the carbonate alone. Temperature-programmed desorption experiments showed that...

  16. Surface science approach to Pt/carbon model catalysts: XPS, STM and microreactor studies

    Science.gov (United States)

    Motin, Abdul Md.; Haunold, Thomas; Bukhtiyarov, Andrey V.; Bera, Abhijit; Rameshan, Christoph; Rupprechter, Günther

    2018-05-01

    Pt nanoparticles supported on carbon are an important technological catalyst. A corresponding model catalyst was prepared by physical vapor deposition (PVD) of Pt on sputtered HOPG (highly oriented pyrolytic graphite). The carbon substrate before and after sputtering as well as the Pt/HOPG system before and after Pt deposition and annealing were examined by XPS and STM. This yielded information on the surface density of defects, which serve as nucleation centres for Pt, and on the size distribution (mean size/height) of the Pt nanoparticles. Two different model catalysts were prepared with mean sizes of 2.0 and 3.6 nm, both turned out to be stable upon UHV-annealing to 300 °C. After transfer into a UHV-compatible flow microreactor and subsequent cleaning in UHV and under mbar pressure, the catalytic activity of the Pt/HOPG model system for ethylene hydrogenation was examined under atmospheric pressure flow conditions. This enabled to determine temperature-dependent conversion rates, turnover frequencies (TOFs) and activation energies. The catalytic results obtained are in line with the characteristics of technological Pt/C, demonstrating the validity of the current surface science based model catalyst approach.

  17. Growth of carbon nanocone arrays on a metal catalyst: The effect of carbon flux ionization

    International Nuclear Information System (INIS)

    Levchenko, I.; Khachan, J.; Vladimirov, S. V.; Ostrikov, K.

    2008-01-01

    The growth of carbon nanocone arrays on metal catalyst particles by deposition from a low-temperature plasma is studied by multiscale Monte Carlo/surface diffusion numerical simulation. It is demonstrated that the variation in the degree of ionization of the carbon flux provides an effective control of the growth kinetics of the carbon nanocones, and leads to the formation of more uniform arrays of nanostructures. In the case of zero degree of ionization (neutral gas process), a width of the distribution of nanocone heights reaches 360 nm with the nanocone mean height of 150 nm. When the carbon flux of 75% ionization is used, the width of the distribution of nanocone heights decreases to 100 nm, i.e., by a factor of 3.6. A higher degree of ionization leads to a better uniformity of the metal catalyst saturation and the nanocone growth, thus contributing to the formation of more height-uniform arrays of carbon nanostructures.

  18. Effects of preparation method and active metal content on of Ni/kieselguhr catalyst activity

    International Nuclear Information System (INIS)

    Galuh Widiyarti; Wuryaningsih Sri Rahayu

    2010-01-01

    The preparation and the active metal content influence the activity of catalyst. Study has been conducted to see the activity of Ni/kieselguhr based on preparation method and Nickel (Ni) contents in the catalyst in the laboratory scale. The Ni/kieselguhr catalyst were prepared by impregnation and precipitation methods, with Ni active contents of 10, 20, and 30 % by weight. The catalysts characterization was analyzed using X-Ray Diffraction (XRD). Catalysts activities were analyzed based on decreasing of iodine number from hydrogenation of crude palm oil for 2 hours. The activity tests results show that precipitation catalysts are more active than impregnation catalysts. The decreasing in iodine number of fatty acid after 2 hours of hydrogenation process using precipitation catalysts and impregnation catalysts are 51.53 and 21.85 %, respectively. In addition, the catalysts are more active with increasing Ni contents. (author)

  19. Characterization and evaluation of Pt-Ru catalyst supported on multi-walled carbon nanotubes by electrochemical impedance

    Energy Technology Data Exchange (ETDEWEB)

    Ocampo, A.L.; Miranda-Hernandez, M.; Sebastian, P.J. [Centro de Investigacion en Energia-UNAM, Temixco, 62580 Morelos (Mexico); Morgado, J.; Montoya, J.A. [IMP, Eje Central Lazaro Cardenas 152, 07730 D.F. Mexico (Mexico)

    2006-10-06

    In this work the authors present the results of a systematic characterization and evaluation of the carbon nanotube supported Pt-Ru (Pt-Ru/CNT) for its use as methanol oxidation catalyst. Its activity was compared with that of Pt and Pt-Ru catalysts supported on Vulcan and synthesized from carbonyl precursors, and another commercial Pt-Ru catalyst. The cyclic voltammetry, CO stripping and electrochemical impedance techniques were employed to determine the electrocatalytic activity of the catalysts. The electrochemical studies were performed in 0.5M H{sub 2}SO{sub 4} containing different concentrations of methanol (0.05-1M). The results showed a noticeable influence of the catalyst support (CNT) on the performance of the catalyst for CO oxidation. The electrochemical impedance studies allowed us to separate the different steps in the methanol oxidation reaction and to control these steps or reactions by varying the applied potential and the methanol concentration. At low methanol concentration and potentials the de-hydrogenation of methanol predominated. But, at high potential and methanol concentrations, the CO oxidation predominated. These results allowed us to clearly describe at what potential and concentration ranges the bi-functional effect of Ru becomes evident. Our results indicated that the CO oxidation occurs both on Pt and Ru. Compared to other catalysts, Pt-Ru supported on carbon nanotubes showed superior catalytic activity for CO and methanol oxidation. (author)

  20. 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.

  1. Synthesis of vertical MnO_2 wire arrays on hemp-derived carbon for efficient and robust green catalysts

    International Nuclear Information System (INIS)

    Yang, MinHo; Kim, Dong Seok; Sim, Jae-Wook; Jeong, Jae-Min; Kim, Do Hyun; Choi, Jae Hyung; Kim, Jinsoo; Kim, Seung-Soo; Choi, Bong Gill

    2017-01-01

    Highlights: • The three-dimensional nanocomposites based on vertical MnO_2 array on hemp-derived carbon (HDC) were prepared by hydrothermal method. • The 3D v-MnO_2/HDC nanocomposites showed well-defined porous nature with a high specific surface area of 382.3 m"2 g"−"1. • PET glycolysis was performed using the 3D v-MnO_2/HDC nanocomposites as a catalyst, leading to efficient catalytic performance. - Abstract: Three-dimensional (3D) carbon materials derived from waste biomass have been attracted increasing attention in catalysis and materials science because of their great potential of catalyst supports with respect to multi-functionality, unique structures, high surface area, and low cost. Here, we present a facile and efficient way for preparing 3D heterogeneous catalysts based on vertical MnO_2 wires deposited on hemp-derived 3D porous carbon. The 3D porous carbon materials are fabricated by carbonization and activation processes using hemp (Cannabis Sttiva L.). These 3D porous carbon materials are employed as catalyst supports for direct deposition of vertical MnO_2 wires using a one-step hydrothermal method. The XRD and XPS results reveal the crystalline structure of α-MnO_2 wires. The resultant composites are further employed as a catalyst for glycolysis of poly(ethylene terephthalate) (PET) with high conversion yield of 98%, which is expected to be expressly profitable for plastics recycling industry.

  2. Revisiting the electrochemical oxidation of ammonia on carbon-supported metal nanoparticle catalysts

    International Nuclear Information System (INIS)

    Li, Zhe-Fei; Wang, Yuxuan; Botte, Gerardine G.

    2017-01-01

    Highlights: • A procedure to pretreat electrocatalysts to study the ammonia oxidation is provided. • N ads and O/OH ads were identified as the major deactivation species that prevent ammonia oxidatoin. • The electrocatalytic activity, thermodynamics, and possible deactivation mechanisms for ammonia oxidation were elucidated. • The onset potential for ammonia oxidation is related to the hydrogen binding energy of the catalyst. • Ammonia electro-oxidation involves a complex decoupled electron and proton transfer process. - Abstract: The ammonia electro-oxidation reaction (AOR) has been studied due to its promising applications in ammonia electrolysis, wastewater remediation, direct ammonia fuel cells, and sensors. However, it is difficult to compare and analyze the reported electrocatalytic activity of AOR reliably, likely due to the variation in catalyst synthesis, electrode composition, electrode morphology, and testing protocol. In this paper, the electro-oxidation of ammonia on different carbon-supported precious metal nanoparticle catalysts was revisited. The effect of experimental conditions, electrochemical test parameters, electrocatalytic activity, thermodynamics, and possible deactivation mechanism of the catalysts were investigated. Pt/C catalyst possesses the highest electrocatalytic activity, while Ir/C and Rh/C show lower overpotential. The onset potential of the AOR is related to the hydrogen binding energy of the catalyst. N ads is one major cause of deactivation accompanied with the formation of surface O/OH ads at high potentials. The coulombic efficiency of N ads formation on Pt is about 1% initially and gradually decreases with reaction time. Increase in ammonia concentration leads to increase in current density, while increase in hydroxyl ions concentration can enhance the current density and reduce the overpotential simultaneously. The slopes of AOR onset potential and hydrogen adsorption/desorption potential of Pt/C as a function of p

  3. Hydrogenation of carbon monoxide on WO/sub 3/-Supported ruthenium catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Yoshinari, Tomohiro; Suganuma, Fujio; Sera, Chikara

    1988-01-01

    In this study, a WO/sub 3/-supported catalyst was prepared to conduct hydrogenation of CO for examining the product distribution and composition of hydrocarbons, using a gamma-alumina-supported catalyst for comparison. These catalysts were used under pressure to conduct a distributive reaction and the desorbing behavior of CO or H/sub 2/ at elevated temperature was measured to examine the influence of the type of carrier or the method of preparation on the activity and the distribution of products formed. The WO/sub 3/-supported catalyst gave a carbon chain length distribution that did not comply with the rule of Schulz-Flory, giving a composition richer in the isomers. Carbon number distribution is affected by Ru-dispersion, and the selectivity of isomers depends on the acidity of the carrier. Formed products distribution of the WO/sub 3/-supported reaction is attributable to the secondary reaction, which relates to the acidic point of the carrier, of the primary product formed on the metal. (7 figs, 4 tabs, 18 refs)

  4. Development of CuxFe/Al2O3 catalysts for the hydrogenation of carbon monoxide guided by magnetic methods, Moessbauer and infrared spectroscopy

    International Nuclear Information System (INIS)

    Boellaard, E.; Geus, J.W.; Bruggen, J.M. van; Kraan, A.M. van der

    1993-01-01

    A copper-iron catalyst for the hydrogenation of carbon monoxide has been prepared using a supported stoichiometric cyanide complex. Conversion of the cyanide precursor to a metallic catalyst appeared to be a precious process. Copper and iron in the bimetallic particles easily separate by thermal treatment and upon exposure to carbon monoxide, as revealed from Moessbauer and infrared spectroscopy. During Fischer-Tropsch reaction the catalyst exhibits a rapid decline of activity. Magnetisation measurements on spent catalysts indicate that the deactivation is caused by a fast conversion of metallic iron to initially unstable carbides which transform ultimately to more stable carbides. (orig.)

  5. Renewable hydrogen: carbon formation on Ni and Ru catalysts during ethanol steam-reforming

    DEFF Research Database (Denmark)

    Rass-Hansen, Jeppe; Christensen, Christina Hviid; Sehested, J.

    2007-01-01

    for the production of hydrogen is investigated, along with quantitative and qualitative determinations of carbon formation on the catalysts by TPO and TEM experiments. A Ru/ MgAl2O4 catalyst, a Ni/MgAl2O4 catalyst as well as Ag-and K-promoted Ni/ MgAl2O4 catalysts were studied. The operating temperature was between...... addition was a rapid deactivation of the catalyst due to an enhanced gum carbon formation on the Ni crystals. Contrary to this, the effect of K addition was a prolonged resistance against carbon formation and therefore against deactivation. The Ru catalyst operates better than all the Ni catalysts...

  6. 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.

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

    International Nuclear Information System (INIS)

    Arthur, Ernest Evans; Li, Fang; Momade, Francis W.Y.; Kim, Hern

    2014-01-01

    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

  8. Structure and catalytic activity of regenerated spent hydrotreating catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Kim, C.S.; Massoth, F.E.; Furimsky, E. (Utah University, Salt Lake City, UT (USA). Dept. of Fuels Engineering)

    1992-11-01

    Two spent catalysts, obtained from different hydrodemetallation operations, were regenerated by two different treatments, viz. 2% (V/V) O[sub 2]/N[sub 2] and air. One spent catalyst (B), contained 3 wt% V and 15 wt% C, while the other (H) contained 10 wt% V, 14 wt% C and 8 wt% Fe. After regeneration in the O[sub 2]/N[sub 2] stream, catalyst B showed essentially complete recovery of its original surface area, whereas catalyst H showed only 70% recovery. Both catalysts showed substantial losses in surface area by the air treatment. Catalytic activity tests on the regenerated catalysts for hydrodesulfurization of thiophene and for hydrogenation of 1-hexene showed low recovery of activities, even for the regenerated catalyst in which the surface area had been completely recovered. X-ray diffraction analyses of the spent-regenerated catalysts revealed substantial changes in catalyst structure. Surface area and catalytic activity results were qualitatively explained by these catalyst structural changes. 17 refs., 1 fig., 3 tabs.

  9. Ionic liquids as transesterification catalysts: applications for the synthesis of linear and cyclic organic carbonates

    Directory of Open Access Journals (Sweden)

    Maurizio Selva

    2016-08-01

    Full Text Available The use of ionic liquids (ILs as organocatalysts is reviewed for transesterification reactions, specifically for the conversion of nontoxic compounds such as dialkyl carbonates to both linear mono-transesterification products or alkylene carbonates. An introductory survey compares pros and cons of classic catalysts based on both acidic and basic systems, to ionic liquids. Then, innovative green syntheses of task-specific ILs and their representative applications are introduced to detail the efficiency and highly selective outcome of ILs-catalyzed transesterification reactions. A mechanistic hypothesis is discussed by the concept of cooperative catalysis based on the dual (electrophilic/nucleophilic activation of reactants.

  10. A review of carbon-based and non-carbon-based catalyst supports for the selective catalytic reduction of nitric oxide.

    Science.gov (United States)

    Anthonysamy, Shahreen Binti Izwan; Afandi, Syahidah Binti; Khavarian, Mehrnoush; Mohamed, Abdul Rahman Bin

    2018-01-01

    Various types of carbon-based and non-carbon-based catalyst supports for nitric oxide (NO) removal through selective catalytic reduction (SCR) with ammonia are examined in this review. A number of carbon-based materials, such as carbon nanotubes (CNTs), activated carbon (AC), and graphene (GR) and non-carbon-based materials, such as Zeolite Socony Mobil-5 (ZSM-5), TiO 2 , and Al 2 O 3 supported materials, were identified as the most up-to-date and recently used catalysts for the removal of NO gas. The main focus of this review is the study of catalyst preparation methods, as this is highly correlated to the behaviour of NO removal. The general mechanisms involved in the system, the Langmuir-Hinshelwood or Eley-Riedeal mechanism, are also discussed. Characterisation analysis affecting the surface and chemical structure of the catalyst is also detailed in this work. Finally, a few major conclusions are drawn and future directions for work on the advancement of the SCR-NH 3 catalyst are suggested.

  11. High activity PtRu/C catalysts synthesized by a modified impregnation method for methanol electro-oxidation

    International Nuclear Information System (INIS)

    Ma Liang; Liu Changpeng; Liao Jianhui; Lu Tianhong; Xing Wei; Zhang Jiujun

    2009-01-01

    A modified impregnation method was used to prepare highly dispersive carbon-supported PtRu catalyst (PtRu/C). Two modifications to the conventional impregnation method were performed: one was to precipitate the precursors ((NH 4 ) 2 PtCl 6 and Ru(OH) 3 ) on the carbon support before metal reduction; the other was to add a buffer into the synthetic solution to stabilize the pH. The prepared catalyst showed a much higher activity for methanol electro-oxidation than a catalyst prepared by the conventional impregnation method, even higher than that of current commercially available, state-of-the-art catalysts. The morphology of the prepared catalyst was characterized using TEM and XRD measurements to determine particle sizes, alloying degree, and lattice parameters. Electrochemical methods were also used to ascertain the electrochemical active surface area and the specific activity of the catalyst. Based on XPS measurements, the high activity of this catalyst was found to originate from both metallic Ru (Ru 0 ) and hydrous ruthenium oxides (RuO x H y ) species on the catalyst surface. However, RuO x H y was found to be more active than metallic Ru. In addition, the anhydrous ruthenium oxide (RuO 2 ) species on the catalyst surface was found to be less active.

  12. Carbonized tantalum catalysts for catalytic chemical vapor deposition of silicon films

    Energy Technology Data Exchange (ETDEWEB)

    Cheng Shimin [State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Dalian National Laboratory for Clean Energy, Dalian 116023 (China); Graduate University of Chinese Academy of Sciences, Beijing 100049 (China); Gao Huiping; Ren Tong; Ying Pinliang [State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Dalian National Laboratory for Clean Energy, Dalian 116023 (China); Li Can, E-mail: canli@dicp.ac.cn [State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Dalian National Laboratory for Clean Energy, Dalian 116023 (China)

    2012-06-01

    Catalytic chemical vapor deposition (Cat-CVD) has been demonstrated as a promising way to prepare device-quality silicon films. However, catalyst ageing due to Si contamination is an urgency to be solved for the practical application of the technique. In this study, the effect of carbonization of tantalum catalyst on its structure and performance was investigated. The carbonized Ta catalyst has a TaC surface layer which is preserved over the temperature range between 1450 and 1750 Degree-Sign C and no Si contamination occurs on the catalyst after long-term use. Si film prepared using the carbonized Ta catalyst has a similar crystal structure to that prepared by uncarbonized Ta catalyst. Formation of the TaC surface layer can alleviate the ageing problem of the catalyst, which shows great potential as a stable catalyst for Cat-CVD of Si films. - Highlights: Black-Right-Pointing-Pointer Si films prepared by catalytic chemical vapor deposition. Black-Right-Pointing-Pointer Carbonized Ta with a TaC surface layer used as catalyst. Black-Right-Pointing-Pointer TaC surface structure preserved after long-term use in a wide temperature range. Black-Right-Pointing-Pointer Help to solve the ageing problem of metal catalysts. Black-Right-Pointing-Pointer Si film obtained has a similar crystal structure to that prepared by Ta catalyst.

  13. Activation of molecular catalysts using semiconductor quantum dots

    Science.gov (United States)

    Meyer, Thomas J [Chapel Hill, NC; Sykora, Milan [Los Alamos, NM; Klimov, Victor I [Los Alamos, NM

    2011-10-04

    Photocatalytic materials based on coupling of semiconductor nanocrystalline quantum dots (NQD) and molecular catalysts. These materials have capability to drive or catalyze non-spontaneous chemical reactions in the presence of visible radiation, ultraviolet radiation, or both. The NQD functions in these materials as a light absorber and charge generator. Following light absorption, the NQD activates a molecular catalyst adsorbed on the surface of the NQD via transfer of one or more charges (either electrons or electron-holes) from the NQD to the molecular catalyst. The activated molecular catalyst can then drive a chemical reaction. A photoelectrolytic device that includes such photocatalytic materials is also described.

  14. Heterogeneous Catalysts for VOC Oxidation from Red Mud and Bagasse Ash Carbon

    Science.gov (United States)

    Pande, Gaurav

    A range of VOC oxidation catalysts have been prepared in this study from agricultural and industrial waste as the starting point. The aim is to prepare catalysts with non-noble metal oxides as the active catalytic component (iron in red mud). The same active component was also supported on activated carbon obtained from unburned carbon in bagasse ash. Red mud which is an aluminum industry waste and rich in different phases of iron as oxide and hydroxide is used as the source for the catalytically active species. It is our aim to enhance the catalytic performance of red mud which though high in iron concentration has a low surface area and may not have the properties of an ideal catalyst by itself. In one of the attempts to enhance the catalytic performance, we have tried to leach red mud for which we have explored a range of leaching acids for effecting the leaching most efficiently and then precipitated the iron from the leachate as its hydroxide by precipitating with alkali solution followed by drying and calcination to give high surface area metal oxide material. Extensive surface characterization and VOC oxidation catalytic testing were performed for these solids. In a step to further enhance the catalytic activity towards oxidation, copper was introduced by taking another industrial waste from the copper tubing industry viz. the pickling acid. Copper has a more favourable redox potential making it catalytically more effective than iron. To make the mixed metal oxide, red mud leachate was mixed with the pickling acid in a pre-decided ratio before precipitating with alkali solution followed by drying and calcination as was done with the red mud leachate. The results from these experiments are encouraging. The temperature programmed reduction (TPR) of the solids show that the precipitate of red mud leachates show hydrogen uptake peak at a lower temperature than for just the calcined red mud. This could be due to the greatly enhanced surface area of the prepared

  15. Nitrogen and Fluorine co-doped carbon catalyst with high oxygen reduction performance, prepared by pyrolyzing a mixture of melamine and PTFE

    International Nuclear Information System (INIS)

    Peng, Hongliang; Liu, Fangfang; Qiao, Xiaochang; Xiong, Ziang; Li, Xiuhua; Shu, Ting; Liao, Shijun

    2015-01-01

    Graphical abstract: A novel N and F co-doped metal-free doped carbon catalyst with three dimensional vesicles structures and ultra thin walls are prepared by pyrolyzing the mixture of melamine and PTFE. The catalyst has high N and F contents (13 and 6 at.%), and exhibits high ORR activity, high stability, and high limitation current density in both alkaline and acid medium. - Highlights: • N and F co-doped carbon catalyst was derived from the mixture of PTFE and melamine. • The N and F contents of the catalyst are up to 13 and 6 at.%, respectively. • The catalyst has three dimensional vesicles structure with ultra thin walls. • ORR activity of the catalyst is superior to that of Pt/C catalyst in alkaline medium. - Abstract: A novel nitrogen and fluorine co-doped carbon catalyst (C-Mela-PTFE) is prepared by pyrolyzing a mixture of melamine and polytetrafluoroethylene (PTFE), the catalyst has a three-dimensional vesicular structure with ultrathin wall, and exhibits excellent ORR performance in both alkaline and acidic mediums. In an alkaline medium, the catalyst exhibits superior ORR activity to that of commercial Pt/C catalyst. Notably, the ORR activity of the catalyst is just slightly lower than that of Pt/C catalyst in acidic medium. It is interesting that the ORR limiting current density of our C-Mela-PTFE catalyst is much higher than that of Pt/C catalyst. The effects of the melamine/PTFE ratio and the pyrolysis temperature on the catalyst's ORR performance are investigated. The optimal melamine/PTFE ratio by weight is 1:1.5, and the optimal pyrolysis temperature is 950 °C. The catalyst samples are characterized by XRD, SEM/TEM, Raman analysis, and XPS, the results reveal the ultra-thin-walled vesicular structure, high surface area and porosity, and high doping amounts of N and F of the catalyst. For the optimal sample, the N and F contents are up to 13 and 6 at.%, respectively, the proportion of pyridinic N is up to 45 at.% according to the

  16. Fuels by Waste Plastics Using Activated Carbon, MCM-41, HZSM-5 and Their Mixture

    Directory of Open Access Journals (Sweden)

    Miskolczi Norbert

    2016-01-01

    Full Text Available Waste material was pyrolyzed in a horizontal tubular reactor at 530-540°C using different catalysts, such as activated carbon, MCM-41, HZSM-5 and their mixtures. Products were investigated by gas-chromatography, EDXRFS and standardized methods. Catalysts significantly affected the yields of volatiles; e.g. HZSM-5 catalyst increased especially the yield of gaseous hydrocarbons, while MCM-41 catalyst was responsible for increasing the pyrolysis oil yield. Synergistic effects were found using mixtures of different catalysts. Furthermore the catalysts modified the main carbon frame of the products. Pyrolysis oil obtained over HZSM-5 catalyst contained large amounts of aromatics, while MCM-41 catalyst mainly isomerized the carbon frame. Regarding contaminants it was concluded, that the sulphur content could be significantly decreased by activated carbon, however it had only a slight effect to the other properties of the products.

  17. 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

  18. Stable amorphous georgeite as a precursor to a high-activity catalyst

    Science.gov (United States)

    Kondrat, Simon A.; Smith, Paul J.; Wells, Peter P.; Chater, Philip A.; Carter, James H.; Morgan, David J.; Fiordaliso, Elisabetta M.; Wagner, Jakob B.; Davies, Thomas E.; Lu, Li; Bartley, Jonathan K.; Taylor, Stuart H.; Spencer, Michael S.; Kiely, Christopher J.; Kelly, Gordon J.; Park, Colin W.; Rosseinsky, Matthew J.; Hutchings, Graham J.

    2016-03-01

    Copper and zinc form an important group of hydroxycarbonate minerals that include zincian malachite, aurichalcite, rosasite and the exceptionally rare and unstable—and hence little known and largely ignored—georgeite. The first three of these minerals are widely used as catalyst precursors for the industrially important methanol-synthesis and low-temperature water-gas shift (LTS) reactions, with the choice of precursor phase strongly influencing the activity of the final catalyst. The preferred phase is usually zincian malachite. This is prepared by a co-precipitation method that involves the transient formation of georgeite; with few exceptions it uses sodium carbonate as the carbonate source, but this also introduces sodium ions—a potential catalyst poison. Here we show that supercritical antisolvent (SAS) precipitation using carbon dioxide (refs 13, 14), a process that exploits the high diffusion rates and solvation power of supercritical carbon dioxide to rapidly expand and supersaturate solutions, can be used to prepare copper/zinc hydroxycarbonate precursors with low sodium content. These include stable georgeite, which we find to be a precursor to highly active methanol-synthesis and superior LTS catalysts. Our findings highlight the value of advanced synthesis methods in accessing unusual mineral phases, and show that there is room for exploring improvements to established industrial catalysts.

  19. Catalytic oxidation of albendazole using molybdenum supported on carbon nanotubes as catalyst

    International Nuclear Information System (INIS)

    Sun-Kou, Maria del Rosario; Vega Carrasco, Edgar R.; Picasso Escobar, Gino I.

    2013-01-01

    The catalytic oxidation reaction of the thioether group (-S-) in the structure to the drug albendazole (C 12 H 15 N 3 O 2 S) was studied in order to obtain a pharmacologically active molecule known as albendazole sulfoxide. With this purpose, three heterogeneous catalysts were prepared using molybdenum (Mo) as active phase and carbon nanotubes as a multiple-layer catalyst support. The incorporation of the active phase was performed by wet impregnation, with subsequent calcination for 4 hours at 400 o C. For the catalytic oxidation reaction was employed hydrogen peroxide-urea (H 2 NCONH 2 ·H 2 O 2 ) as oxidizing agent and methanol (CH 3 OH) as reaction medium. The textural and morphology characterization of carbon nanoparticles and catalysts was carried out by adsorption-desorption of N 2 (BET) and scanning electron microscopy (SEM). The identification and quantification of the reaction products were followed by Fourier transform infrared spectroscopy (FTIR) and high performance liquid chromatography (HPLC), respectively. With the yield, selectivity and conversion higher than 90% after 60 minutes of reaction, albendazole sulphoxide was obtained as major product of oxidation reaction. (author)

  20. Carbon activity meter

    International Nuclear Information System (INIS)

    Roy, P.; Krankota, J.L.

    1975-01-01

    A carbon activity meter utilizing an electrochemical carbon cell with gaseous reference electrodes having particular application for measuring carbon activity in liquid sodium for the LMFBR project is described. The electrolyte container is electroplated with a thin gold film on the inside surface thereof, and a reference electrode consisting of CO/CO 2 gas is used. (U.S.)

  1. Synthesis of carbon-supported nickel catalysts for the dry reforming of CH{sub 4}

    Energy Technology Data Exchange (ETDEWEB)

    Fidalgo, B.; Zubizarreta, L.; Bermudez, J.M.; Arenillas, A.; Menendez, J.A. [Instituto Nacional del Carbon, CSIC, Apartado 73, 33080 Oviedo (Spain)

    2010-07-15

    A series of carbon-based nickel (Ni) catalysts was prepared in order to investigate the effect of the preparation method on the dispersion of Ni and its final catalytic activity in the dry reforming of methane, i.e. CH{sub 4} + CO{sub 2} 2H{sub 2} + 2CO. Three parameters were studied: (i) the influence of the surface chemistry of the carbon used as support; (ii) the method of drying (conventional vs. microwave drying); and, (iii) the temperature of the reduction stage. In order to study the role of the surface chemistry of the commercial activated carbon used as support, the active carbon was tested as received and oxidized. Although a better Ni dispersion was achieved over the oxidized support, the conversions were much lower. It was also found that microwave drying offers various advantages over conventional drying, the main one being that less time is required to prepare the catalyst. Two reduction temperatures were used (300 and 500 C), being found that it is necessary to adjust this parameter to prevent the Ni particles from sintering. (author)

  2. Carbon-supported cobalt catalyst for hydrogen generation from alkaline sodium borohydride solution

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Dongyan; Liu, Xinmin; Cao, Changqing; Guo, Qingjie [College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042 (China); Dai, Ping [College of Electromechanical Engineering, Qingdao University of Science and Technology, Qingdao 266061 (China)

    2008-08-01

    Low cost transition metal catalysts with high performance are attractive for the development of on-board hydrogen generation systems by catalytic hydrolysis of sodium borohydride (NaBH{sub 4}) in fuel cell fields. In this study, hydrogen production from alkaline NaBH{sub 4} via hydrolysis process over carbon-supported cobalt catalysts was studied. The catalytic activity of the supported cobalt catalyst was found to be highly dependent on the calcination temperatures. The hydrogen generation rate increases with calcination temperatures in the range of 200-400 C, but a high calcination temperature above 500 C led to markedly decreased activity. X-ray diffraction patterns reveal that the catalysts experience phase transition from amorphous Co-B to crystalline cobalt hydroxide with increase in calcination temperatures. The reaction performance is also dependent on the concentration of NaBH{sub 4}, and the hydrogen generation rate increases for lower NaBH{sub 4} concentrations and decreases after reaching a maximum at 10 wt.% of NaBH{sub 4}. (author)

  3. Activated carbons and gold

    International Nuclear Information System (INIS)

    McDougall, G.J.; Hancock, R.D.

    1980-01-01

    The literature on activated carbon is reviewed so as to provide a general background with respect to the effect of source material and activation procedure on carbon properties, the structure and chemical nature of the surface of the activated carbon, and the nature of absorption processes on carbon. The various theories on the absorption of gold and silver from cyanide solutions are then reviewed, followed by a discussion of processes for the recovery of gold and silver from cyanide solutions using activated carbon, including a comparison with zinc precipitation

  4. Hierarchical nanostructured hollow spherical carbon with mesoporous shell as a unique cathode catalyst support in proton exchange membrane fuel cell.

    Science.gov (United States)

    Fang, Baizeng; Kim, Jung Ho; Kim, Minsik; Kim, Minwoo; Yu, Jong-Sung

    2009-03-07

    Hierarchical nanostructured spherical carbon with hollow macroporous core in combination with mesoporous shell has been explored to support Pt cathode catalyst with high metal loading in proton exchange membrane fuel cell (PEMFC). The hollow core-mesoporous shell carbon (HCMSC) has unique structural characteristics such as large specific surface area and mesoporous volume, ensuring uniform dispersion of the supported high loading (60 wt%) Pt nanoparticles with small particle size, and well-developed three-dimensionally interconnected hierarchical porosity network, facilitating fast mass transport. The HCMSC-supported Pt(60 wt%) cathode catalyst has demonstrated markedly enhanced catalytic activity toward oxygen reduction and greatly improved PEMFC polarization performance compared with carbon black Vulcan XC-72 (VC)-supported ones. Furthermore, the HCMSC-supported Pt(40 wt%) or Pt(60 wt%) outperforms the HCMSC-supported Pt(20 wt%) even at a low catalyst loading of 0.2 mg Pt cm(-2) in the cathode, which is completely different from the VC-supported Pt catalysts. The capability of supporting high loading Pt is supposed to accelerate the commercialization of PEMFC due to the anticipated significant reduction in the amount of catalyst support required, diffusion layer thickness and fabricating cost of the supported Pt catalyst electrode.

  5. 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. Copyright © 2016 Elsevier Ltd. All rights reserved.

  6. CATALYSTS BASED ON UKRAINIAN NATURAL SORBENTS FOR LOW-TEMPERATURE CARBON MONOXIDE OXIDATION MEANT FOR INDIVIDUAL RESPIRATORY PROTECTIVE DEVICES

    Directory of Open Access Journals (Sweden)

    T. L. Rakyts’ka

    2015-11-01

    Full Text Available In spite of a great number of patented formulas of catalysts for neutralization of carbon monoxide (CO which is the most widespread atmospheric pollutant, only batch-produced hopcalite and alumina supported palladium (Pd/Al2O3 are used in practice. The named catalysts have significant defects: hopcalite is poisonable in the presence of water vapor and Pd/Al2O3 is characterized by the great content of palladium. We have found the possibility of using inexpensive Ukrainian natural sorbents differing by their mineralogical and chemical compositions, i.e. zeolites, bentonites, basalt tuffs, and disperse silicas, as supports for development and subsequent application of palladium(II and copper(II based catalysts for carbon monoxide oxidation. Acid-thermally modified Ukrainian sorbents have been found to be proper for obtaining supported copper-palladium complexes the most catalytically active in the reaction. Application of Ukrainian natural tripolis permitted to avoid the step of acid-thermal modification complicating the technique of catalyst production. As was found, the origin and phase composition of tripolis affect the activity of catalysts supported on them in the reaction of low-temperature Co oxidation. The most active catalyst permitting sanitary purification of air from CO to a level permissible for atmosphere of populated areas have been obtained in the case of insignificantly (thermally or hydrothermally modified tripoli from Konoplianskoe deposit.

  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. Development of Sulfur and Carbon Tolerant Reforming Alloy Catalysts Aided by Fundamental Atomistics Insights

    Energy Technology Data Exchange (ETDEWEB)

    Suljo Linic

    2006-08-31

    Current hydrocarbon reforming catalysts suffer from rapid carbon and sulfur poisoning. Even though there is a tremendous incentive to develop more efficient catalysts, these materials are currently formulated using inefficient trial and error experimental approaches. We have utilized a novel hybrid experimental/theoretical approach, combining quantum Density Functional Theory (DFT) calculations and various state-of-the-art experimental tools, to formulate carbon tolerant reforming catalysts. We have employed DFT calculations to develop molecular insights into the elementary chemical transformations that lead to carbon poisoning of Ni catalysts. Based on the obtained molecular insights, we have identified, using DFT quantum calculation, Sn/Ni alloy as a potential carbon tolerant reforming catalyst. Sn/Ni alloy was synthesized and tested in steam reforming of methane, propane, and isooctane. We demonstrated that the alloy catalyst is carbon-tolerant under nearly stoichiometric steam-to-carbon ratios. Under these conditions, monometallic Ni is rapidly poisoned by sp2 carbon deposits. The research approach is distinguished by a few characteristics: (a) Knowledge-based, bottom-up approach, compared to the traditional trial and error approach, allows for a more efficient and systematic discovery of improved catalysts. (b) The focus is on exploring alloy materials which have been largely unexplored as potential reforming catalysts.

  9. Activity Tests of Macro-Meso Porous Catalysts over Metal Foam Plate for Steam Reforming of Bio-Ethanol.

    Science.gov (United States)

    Park, No-Kuk; Jeong, Yong Han; Kang, Misook; Lee, Tae Jin

    2018-09-01

    The catalytic activity of a macro-mesoporous catalyst coated on a metal foam plate in the reforming of bio-ethanol to synthesis gas was investigated. The catalysts were prepared by coating a support with a noble metal and transition metal. The catalytic activity for the production of synthetic gas by the reforming of bio-ethanol was compared according to the support material, reaction temperature, and steam/carbon ratio. The catalysts coated on the metal foams were prepared using a template method, in which macro-pores and meso-pores were formed by mixing polymer beads. In particular, the thermodynamic equilibrium composition of bio-ethanol reforming with the reaction temperature and steam/carbon ratio to produce synthetic gas was examined using the HSC (Enthalpy-Entropy-Heat capacity) chemistry program in this study. The composition of hydrogen and carbon monoxide in the reformate gas produced by steam reforming over the Rh/Ni-Ce-Zr/Al2O3-based pellet type catalysts and metal foam catalysts that had been coated with the Rh/Al-Ce-Zr-based catalysts was investigated by experimental activity tests. The activity of the metal foam catalyst was higher than that of the pellet type catalyst.

  10. Fuel cell testing of Pt–Ru catalysts supported on differently prepared and pretreated carbon nanotubes

    International Nuclear Information System (INIS)

    Tokarz, Wojciech; Lota, Grzegorz; Frackowiak, Elzbieta; Czerwiński, Andrzej; Piela, Piotr

    2013-01-01

    Proton-exchange membrane fuel cell (PEMFC) testing of Pt–Ru catalysts supported on differently prepared multiwall carbon nanotube (MCNT) supports was performed to elucidate the influence of the different supports on the operating characteristics of the catalysts under real direct methanol fuel cell (DMFC) anode and H 2 -PEMFC anode conditions. The MCNTs were either thin, entangled or thick, disentangled. Pretreatment of the MCNTs was also done and it was either high-temperature KOH etching or annealing (graphitization). The performance of the catalysts was compared against the performance of a commercial Pt–Ru catalyst supported on a high-surface-area carbon black. Among the different MCNT supports, the graphitized, entangled support offered the best performance in all tests, which was equal to the performance of the commercial catalyst, despite the MCNT catalyst layer was ca. 2.2 times thicker than the carbon black catalyst layer. Even for an MCNT catalyst layer, which was almost 7 times thicker than the carbon black catalyst layer, the transport limitations were not prohibitive. This confirmed the expected potential of nanotube supports for providing superior reactant transport properties of the PEMFC catalyst layers

  11. Large-scale synthesis of coiled-like shaped carbon nanotubes using bi-metal catalyst

    Science.gov (United States)

    Krishna, Vemula Mohana; Somanathan, T.; Manikandan, E.; Umar, Ahmad; Maaza, M.

    2018-02-01

    Carbon nanomaterials (CNMs), especially carbon nanotubes (CNTs) with coiled structure exhibit scientifically fascinating. They may be projected as an innovative preference to future technological materials. Coiled carbon nanotubes (c-CNTs) on a large-scale were successfully synthesized with the help of bi-metal substituted α-alumina nanoparticles catalyst via chemical vapor deposition (CVD) technique. Highly spring-like carbon nanostructures were observed by field emission scanning electron microscope (FESEM) examination. Furthermore, the obtained material has high purity, which correlates the X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDX) analysis. Raman spectroscopy reveals that the carbon multi layers are well graphitized and crystalline, even if they have defects in its structure due to coiled morphology. High-resolution transmission electron microscope (HRTEM) describes internal structure and dia of the product. Ultimately, results support the activity of bi-metal impregnated α-alumina nanoparticles catalyst to determine the high yield, graphitization and internal structure of the material. We have also studied the purified c-CNTs magnetic properties at room temperature and will be an added advantage in several applications.

  12. Activated carbon from biomass

    Science.gov (United States)

    Manocha, S.; Manocha, L. M.; Joshi, Parth; Patel, Bhavesh; Dangi, Gaurav; Verma, Narendra

    2013-06-01

    Activated carbon are unique and versatile adsorbents having extended surface area, micro porous structure, universal adsorption effect, high adsorption capacity and high degree of surface reactivity. Activated carbons are synthesized from variety of materials. Most commonly used on a commercial scale are cellulosic based precursors such as peat, coal, lignite wood and coconut shell. Variation occurs in precursors in terms of structure and carbon content. Coir having very low bulk density and porous structure is found to be one of the valuable raw materials for the production of highly porous activated carbon and other important factor is its high carbon content. Exploration of good low cost and non conventional adsorbent may contribute to the sustainability of the environment and offer promising benefits for the commercial purpose in future. Carbonization of biomass was carried out in a horizontal muffle furnace. Both carbonization and activation were performed in inert nitrogen atmosphere in one step to enhance the surface area and to develop interconnecting porosity. The types of biomass as well as the activation conditions determine the properties and the yield of activated carbon. Activated carbon produced from biomass is cost effective as it is easily available as a waste biomass. Activated carbon produced by combination of chemical and physical activation has higher surface area of 2442 m2/gm compared to that produced by physical activation (1365 m2/gm).

  13. Nitrogen–doped graphitized carbon shell encapsulated NiFe nanoparticles: A highly durable oxygen evolution catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Du, Lei; Luo, Langli; Feng, Zhenxing; Engelhard, Mark; Xie, Xiaohong; Han, Binghong; Sun, Junming; Zhang, Jianghao; Yin, Geping; Wang, Chongmin; Wang, Yong; Shao, Yuyan

    2017-09-01

    Oxygen evolution reaction (OER) plays a crucial role in various energy conversion devices such as water electrolyzers and metal–air batteries. Precious metal catalysts such as Ir, Ru and their oxides are usually used for enhanced reaction kinetics but are limited by their scarce resource. The challenges associated with alternative non–precious metal catalysts such as transition metal oxides and (oxy)hydroxides etc. are their low electronic conductivity and poor durability. Here, we report OER catalysts of NiFe nanoparticles encapsulated by nitrogen–doped graphitized carbon shells derived from bimetallic metal–organic frameworks (MOFs) precursors. The optimal OER catalyst shows excellent activity (360 mV overpotential at 10 mA cm–2GEO) and durability (no obvious degradation after 20 000 cycles). The electron-donation from Fe and tuned electronic structure of metal cores by Ni are revealed to be primary contributors to the enhanced OER activity. We further demonstrated that the structure and morphology of encapsulating carbon shells, which are the key factors influencing the durability, are facilely controlled by chemical state of precursors. Severe metal particle growth probably caused by oxidation of carbon shells and encapsulated nanoparticles is believed to the main mechanism for activity degradation in these catalysts.

  14. Synthesis of carbon-supported copper catalyst and its catalytic performance in methanol dehydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Shelepova, Ekaterina V. [Boreskov Institute of Catalysis SB RAS, pr. Ac. Lavrentieva, 5, Novosibirsk, 630090 (Russian Federation); National Research Tomsk Polytechnic University, Lenin av., 30, Tomsk, 634050 (Russian Federation); Vedyagin, Aleksey A., E-mail: vedyagin@catalysis.ru [Boreskov Institute of Catalysis SB RAS, pr. Ac. Lavrentieva, 5, Novosibirsk, 630090 (Russian Federation); National Research Tomsk Polytechnic University, Lenin av., 30, Tomsk, 634050 (Russian Federation); Ilina, Ludmila Yu.; Nizovskii, Alexander I. [Boreskov Institute of Catalysis SB RAS, pr. Ac. Lavrentieva, 5, Novosibirsk, 630090 (Russian Federation); Tsyrulnikov, Pavel G. [Institute of Hydrocarbon Processing SB RAS, Neftezavodskaya st., 54, Omsk, 644040 (Russian Federation)

    2017-07-01

    Highlights: • Carbon-supported copper catalyst was studied in dehydrogenation of methanol. • Reduction temperature affected size of Cu particles and Cu{sup 0}/Cu{sup 2+} ratio. • Reduction at 400 °C was required to obtain high methyl formate yield. - Abstract: Carbon-supported copper catalyst was prepared by incipient wetness impregnation of Sibunit with an aqueous solution of copper nitrate. Copper loading was 5 wt.%. Temperature of reductive pretreatment was varied within a range of 200–400 °C. The samples were characterized by transmission electron microscopy, X-ray diffraction analysis, X-ray photoelectron and X-ray absorption spectroscopies. Catalytic activity of the samples was studied in a reaction of methanol dehydrogenation. Silica-based catalyst with similar copper loading was used as a reference. It was found that copper is distributed over the surface of support in the form of metallic and partially oxidized particles of about 12–17 nm in size. Diminished interaction of copper with support was supposed to be responsible for high catalytic activity.

  15. Surface treated carbon catalysts produced from waste tires for fatty acids to biofuel conversion

    Science.gov (United States)

    Hood, Zachary D.; Adhikari, Shiba P.; Wright, Marcus W.; Lachgar, Abdessadek; Li, Yunchao; Naskar, Amit K.; Paranthaman, Mariappan Parans

    2018-02-06

    A method of making solid acid catalysts includes the step of sulfonating waste tire pieces in a first sulfonation step. The sulfonated waste tire pieces are pyrolyzed to produce carbon composite pieces having a pore size less than 10 nm. The carbon composite pieces are then ground to produce carbon composite powders having a size less than 50 .mu.m. The carbon composite particles are sulfonated in a second sulfonation step to produce sulfonated solid acid catalysts. A method of making biofuels and solid acid catalysts are also disclosed.

  16. Carbon coated (carbonous) catalyst in ebullated bed reactor for production of oxygenated chemicals from syngas/CO2

    International Nuclear Information System (INIS)

    Peizheng Zhou

    2002-01-01

    This report summarizes the work completed under DOE's Support of Advanced Fuel Research program, Contract No. DE-FG26-99FT40681. The contract period was October 2000 through September 2002. This R and D program investigated the modification of the mechanical strength of catalyst extrudates using Hydrocarbon Technologies, Inc. (HTI) carbon-coated catalyst technology so that the ebullated bed technology can be utilized to produce valuable oxygenated chemicals from syngas/CO 2 efficiently and economically. Exothermic chemical reactions benefit from the temperature control and freedom from catalyst fouling provided by the ebullated bed reactor technology. The carbon-coated extrudates prepared using these procedures had sufficient attrition resistance and surface area for use in ebullated bed operation. The low cost of carbon coating makes the carbon-coated catalysts highly competitive in the market of catalyst extrudates

  17. EXAFS Determination of the Structure of Cobalt in Carbon-Supported Cobalt and Cobalt-Molybdenum Sulfide Hydrodesulfurization Catalysts.

    NARCIS (Netherlands)

    Koningsberger, D.C.; Bouwens, S.M.A.M.; Veen, J.A.R. van; Beer, V.H.J. de; Prins, R.

    1991-01-01

    The structure of the cobalt present in carbon-supported Co and Co-Mo sulfide catalysts was studied by means of X-ray absorption spectroscopy at the Co K-edge and by X-ray photoelectron spectroscopy (XPS). Thiophene hydrodesulfurization activities were used to measure the catalytic properties of

  18. 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

  19. Pt-Fe catalyst nanoparticles supported on single-wall carbon nanotubes: Direct synthesis and electrochemical performance for methanol oxidation

    Science.gov (United States)

    Ma, Xiaohui; Luo, Liqiang; Zhu, Limei; Yu, Liming; Sheng, Leimei; An, Kang; Ando, Yoshinori; Zhao, Xinluo

    2013-11-01

    Single-wall carbon nanotubes (SWCNTs) supported Pt-Fe nanoparticles have been prepared by one-step hydrogen arc discharge evaporation of carbon electrode containing both Pt and Fe metal elements. The formation of SWCNTs and Pt-Fe nanoparticles occur simultaneously during the evaporation process. High-temperature hydrogen treatment and hydrochloric acid soaking have been carried out to purify and activate those materials in order to obtain a new type of Pt-Fe/SWCNTs catalyst for methanol oxidation. The Pt-Fe/SWCNTs catalyst performs much higher electrocatalytic activity for methanol oxidation, better stability and better durability than a commercial Pt/C catalyst according to the electrochemical measurements, indicating that it has a great potential for applications in direct methanol fuel cells.

  20. Electrocatalytic activity mapping of model fuel cell catalyst films using scanning electrochemical microscopy

    International Nuclear Information System (INIS)

    Nicholson, P.G.; Zhou, S.; Hinds, G.; Wain, A.J.; Turnbull, A.

    2009-01-01

    Scanning electrochemical microscopy has been employed to spatially map the electrocatalytic activity of model proton exchange membrane fuel cell (PEMFC) catalyst films towards the hydrogen oxidation reaction (the PEMFC anode reaction). The catalyst films were composed of platinum-loaded carbon nanoparticles, similar to those typically used in PEMFCs. The electrochemical characterisation was correlated with a detailed physical characterisation using dynamic light scattering, transmission electron microscopy and field-emission scanning electron microscopy. The nanoparticles were found to be reasonably mono-dispersed, with a tendency to agglomerate into porous bead-type structures when spun-cast. The number of carbon nanoparticles with little or no platinum was surprisingly higher than would be expected based on the platinum-carbon mass ratio. Furthermore, the platinum-rich carbon particles tended to agglomerate and the clusters formed were non-uniformly distributed. This morphology was reflected in a high degree of heterogeneity in the film activity towards the hydrogen oxidation reaction.

  1. N, S co-doped carbon spheres with highly dispersed CoO as non-precious metal catalyst for oxygen reduction reaction

    Science.gov (United States)

    Chen, Linlin; Guo, Xingpeng; Zhang, Guoan

    2017-08-01

    It is still a great challenge in preparing non-precious metal catalysts with high activity and long-term stability to substitute for precious metal catalysts for oxygen reduction reaction (ORR) in fuel cells. Herein, we report a novel and facile catalyst-N, S co-doped carbon spheres with highly dispersed CoO (CoO@NS-CSs), where biomass glucose spheres act as carbon precursor and H2S, NH3 derived from the decomposition of thiourea not only provide N, S sources but also can etch carbon spheres to produce nanoporous structure. CoO@NS-CSs catalyst exhibits excellent ORR activity with a high onset potential of 0.946 V vs. RHE (reversible hydrogen electrode) and a half-wave potential of 0.821 V vs. RHE through a four-electron pathway in alkaline solution, which is comparable to commercial Pt/C catalyst (onset potential: 0.926 V vs. RHE, half-wave potential: 0.827 V vs. RHE). Furthermore, both the long-term stability and methanol-tolerance of CoO@NS-CSs catalyst are superior to those of commercial Pt/C catalyst. The excellent ORR performance of CoO@NS-CSs catalyst can be attributed to its micro-mesopore structure, high specific surface area (667 m2 g-1), and highly dispersed CoO. This work manifests that the obtained CoO@NS-CSs catalyst is promising to be applied to fuel cells.

  2. Sustainable Applications of Magnetic Nano-catalysts and Graphitic Carbon Nitrides (presentation)

    Science.gov (United States)

    Homogeneous catalysts, known for chemo-, regio- and enantioselectivity, have better contact with the reactants but the catalyst separation creates barriers. Heterogeneous systems enable better separation although at the cost of reduction in the availability of active sites. Becau...

  3. 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...... 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...... nanotubes (GMWCNTs), and graphitized carbon nanofibre (CNF), while the Pt/C samples were platinized samples of some of the CNTs and CNFs (Pt/FWCNT, Pt/GMWCNT, and Pt/CNF, respectively) as well as two commercial Pt/CB reference catalysts. Comparative analyses have been performed in order to be able to assess...

  4. Novel, high-activity hydroprocessing catalysts: Iron group phosphides

    Science.gov (United States)

    Wang, Xianqin

    A series of iron, cobalt and nickel transition metal phosphides was synthesized by means of temperature-programmed reduction (TPR) of the corresponding phosphates. The same materials, Fe2P, CoP and NO, were also prepared on a silica (SiO2) support. The phase purity of these catalysts was established by x-ray diffraction (XRD), and the surface properties were determined by N2 BET specific surface area (Sg) measurements and CO chemisorption. The activities of the silica-supported catalysts were tested in a three-phase trickle bed reactor for the simultaneous hydrodenitrogenation (HDN) of quinoline and hydrodesulfurization (HDS) of dibenzothiophene using a model liquid feed at realistic conditions (30 atm, 370°C). The reactivity studies showed that the nickel phosphide (Ni2P/SiO2) was the most active of the catalysts. Compared with a commercial Ni-Mo-S/gamma-Al 2O3 catalyst at the same conditions, Ni2P/silica had a substantially higher HDS activity (100% vs. 76%) and HDN activity (82% vs. 38%). Because of their good hydrotreating activity, an extensive study of the preparation of silica supported nickel phosphides, Ni2P/SiO 2, was carried out. The parameters investigated were the phosphorus content and the weight loading of the active phase. The most active composition was found to have a starting synthesis Ni/P ratio close to 1/2, and the best loading of this sample on silica was observed to be 18 wt.%. Extended x-ray absorption fine structure (EXAFS) and x-ray absorption near edge spectroscopy (XANES) measurements were employed to determine the structures of the supported samples. The main phase before and after reaction was found to be Ni2P, but some sulfur was found to be retained after reaction. A comprehensive scrutiny of the HDN reaction mechanism was also made over the Ni2P/SiO2 sample (Ni/P = 1/2) by comparing the HDN activity of a series of piperidine derivatives of different structure. It was found that piperidine adsorption involved an alpha-H activation

  5. Novel type of carbon-supported catalysts. I.Preparation and characterization

    NARCIS (Netherlands)

    van Doorn, J.; Staugaard, P.; Moulijn, J.A.; Beer, de V.H.J.

    1989-01-01

    The exposure of CoO/Al2O3 catalysts to carbon monoxide leads, after reduction to cobalt metal, to the formation of filamentary carbon in addition to a less reactive form of deposited carbon. The filament diameters were determined by scanning electron microscopy. The carbon content was determined by

  6. The synthesis of carbon nanocomposites as fuel cell catalyst support and the characterization of fuel cell catalysts by spatially resolved scanning mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Li, Nan

    2007-07-01

    Ammonia decomposition over Ni/SiO{sub 2} and Ni/MgO was investigated by temperature-programmed desorption (TPD) and temperature-programmed surface reaction (TPSR) in order to produce CO{sub x} free hydrogen fuel for fuel cell application. A highly efficient route for the synthesis of carbon nanocomposites based on electrochemical deposition and iron catalyzed chemical vapor deposition (CVD) was developed in order to obtain a promising substrate for fuel cell catalysts. The duration of electrochemical deposition, temperature and time for the carbon nanotubes (CNTs) growth had been optimized to achieve higher surface area after the growth. Hierarchically structured CNTs composites had been synthesized and electrochemical studies provided evidence for the strong interaction among the substrate and grown CNTs, which are essential for the application in fuel cells. A straightforward strategy was developed to synthesize well dispersed gold nanoparticles with a diameter of 4 to 6 nm on the sidewall of multi-walled carbon nanotubes (MWNTs). A gas flow set-up was developed for the evaluation of fuel cell catalysts by performing scanning mass spectrometry with integrated constant-distance positioning. Methanol oxidation was identified as a suitable test reaction. The diameter of scanning probe was reduced in order to achieve higher spatial resolution. Spatially resolved scanning mass spectrometry was successfully applied to visualize the catalytic activity over Pt-based catalysts and monitor the local activity of a catalysts coated membrane (CCM). The gas-solid phase reaction results were proved to be accurate, reliable and independent of the sample topography. This analytical method opens the way for fast quality control of the catalyst coating with respect to even coating and absence of damages, and for a better understanding of the CCM degradation in polymer membrane electrolyte fuel cells (PEMFCs). (orig.)

  7. Nitric Oxide Reduction by Carbon Monoxide over Supported Hexaruthenium Cluster Catalysts. 1. The Active Site Structure That Depends on Supporting Metal Oxide and Catalytic Reaction Conditions.

    Science.gov (United States)

    Minato, Taketoshi; Izumi, Yasuo; Aika, Ken-Ichi; Ishiguro, Atsushi; Nakajima, Takayuki; Wakatsuki, Yasuo

    2003-08-28

    Ruthenium site structures supported on metal oxide surfaces were designed by reacting organometallic Ru cluster [Ru6C(CO)16](2-) or [Ru6(CO)18](2-) with various metal oxides, TiO2, Al2O3, MgO, and SiO2. The surface Ru site structure, formed under various catalyst preparation and reaction conditions, was investigated by the Ru K-edge extended X-ray absorption fine structure (EXAFS). Samples of [Ru6C(CO)16](2-)/TiO2(anatase) and [Ru6C(CO)16](2-)/TiO2(rutile) were found to retain the original Ru6C framework when heated in the presence of NO (2.0 kPa) or NO (2.0 kPa) + CO (2.0 kPa) at 423 K, i.e., catalytic reaction conditions for NO decomposition. At 523 K, the Ru-Ru bonds of the Ru6C framework were cleaved by the attack of NO. In contrast, the Ru site became spontaneously dispersed over TiO2 (anatase). When being supported over TiO2 (mesoporous), MgO, or Al2O3, the Ru6C framework split into fragments in gaseous NO or NO + CO even at 423 K. The Ru6 framework of [Ru6(CO)18](2-) was found to break easily into smaller ensembles in the presence of NO and/or CO at 423 K on support. Taking into consideration the realistic environments in which these catalysts will be used, we also examined the effect of water and oxygen. When water was introduced to the sample [Ru6C(CO)16](2-)/TiO2(anatase) at 423 K, it did not have any effects on the stabilized Ru6C framework structure. In the presence of oxygen gas, however, the Ru hexanuclear structure decomposed into isolated Ru cations bound to surface oxygen atoms of TiO2 (anatase).

  8. Experimental research of technology activating catalysts for SCR DeNOx in boiler

    Science.gov (United States)

    Zeng, Xi; Yang, Zhengde; Li, Yan; Chen, Donglin

    2018-01-01

    In order to improve activity of the catalysts used in SCR DeNOx system of flue gas, a series of catalysts activated by different activating liquids under varied conditions in boiler directly were conducted. Then these catalysts were characterized by SEM, FT-IR and BET technology. And NO conversions of the activated catalysts were studied and compared with that of inactivated catalyst. The above experiment shows that NO conversion of the activated catalyst can be up to 99%, which 30% higher than that of inactivated catalyst, so activity of catalysts were improved greatly. Furthermore, optimal activating liquid labeled L2 and effective technology parameters were gained in the experiment.

  9. Patterned growth of carbon nanotubes on Si substrates without predeposition of metal catalysts

    Science.gov (United States)

    Chen, Y.; Yu, J.

    2005-07-01

    Aligned carbon nanotubes (CNTs) can be readily synthesized on quartz or silicon-oxide-coated Si substrates using a chemical vapor deposition method, but it is difficult to grow them on pure Si substrates without predeposition of metal catalysts. We report that aligned CNTs were grown by pyrolysis of iron phthalocyanine at 1000°C on the templates created on Si substrates with simple mechanical scratching. Scanning electron microscopy and x-ray energy spectroscopy analysis revealed that the trenches and patterns created on the surface of Si substrates were preferred nucleation sites for nanotube growth due to a high surface energy, metastable surface structure, and possible capillarity effect. A two-step pyrolysis process maintained Fe as an active catalyst.

  10. Fischer-Tropsch Cobalt Catalyst Activation and Handling Through Wax Enclosure Methods

    Science.gov (United States)

    Klettlinger, Jennifer L. S.; Yen, Chia H.; Nakley, Leah M.; Surgenor, Angela D.

    2016-01-01

    Fischer-Tropsch (F-T) synthesis is considered a gas to liquid process which converts syn-gas, a gaseous mixture of hydrogen and carbon monoxide, into liquids of various hydrocarbon chain length and product distributions. Cobalt based catalysts are used in F-T synthesis and are the focus of this paper. One key concern with handling cobalt based catalysts is that the active form of catalyst is in a reduced state, metallic cobalt, which oxidizes readily in air. In laboratory experiments, the precursor cobalt oxide catalyst is activated in a fixed bed at 350 ?C then transferred into a continuous stirred tank reactor (CSTR) with inert gas. NASA has developed a process which involves the enclosure of active cobalt catalyst in a wax mold to prevent oxidation during storage and handling. This improved method allows for precise catalyst loading and delivery into a CSTR. Preliminary results indicate similar activity levels in the F-T reaction in comparison to the direct injection method. The work in this paper was supported by the NASA Fundamental Aeronautics Subsonics Fixed Wing Project.

  11. In-Situ Liquid Hydrogenation of m-Chloronitrobenzene over Fe-Modified Pt/Carbon Nanotubes Catalysts

    Directory of Open Access Journals (Sweden)

    Feng Li

    2018-02-01

    Full Text Available In-situ liquid-phase hydrogenation of m-chloronitrobenzene (m-CNB based on aqueous-phase reforming (APR of ethanol and catalytic hydrogenation was carried out over Fe-modified Pt/carbon nanotubes (CNTs catalysts. The effects of Pt loading over CNTs and Fe modification on the catalytic performance of Pt/CNTs catalysts were studied. In-tube loading of Pt particles, compared with out-tube loading, considerably improved the catalytic activity. With in-tube loading, Fe-modified Pt/CNTs catalysts further improved the m-CNB in-situ hydrogenation performance. After Fe modification, Pt–Fe/CNTs catalysts formed, inside CNTs, a Pt–Fe alloy and iron oxides, which both improved catalytic hydrogenation performance and significantly enhanced ethanol APR hydrogen producing performance, thereby increasing the m-CNB in-situ hydrogenation reactivity.

  12. Highly efficient nonprecious metal catalyst prepared with metal–organic framework in a continuous carbon nanofibrous network

    Science.gov (United States)

    Shui, Jianglan; Chen, Chen; Grabstanowicz, Lauren; Zhao, Dan; Liu, Di-Jia

    2015-01-01

    Fuel cell vehicles, the only all-electric technology with a demonstrated >300 miles per fill travel range, use Pt as the electrode catalyst. The high price of Pt creates a major cost barrier for large-scale implementation of polymer electrolyte membrane fuel cells. Nonprecious metal catalysts (NPMCs) represent attractive low-cost alternatives. However, a significantly lower turnover frequency at the individual catalytic site renders the traditional carbon-supported NPMCs inadequate in reaching the desired performance afforded by Pt. Unconventional catalyst design aiming at maximizing the active site density at much improved mass and charge transports is essential for the next-generation NPMC. We report here a method of preparing highly efficient, nanofibrous NPMC for cathodic oxygen reduction reaction by electrospinning a polymer solution containing ferrous organometallics and zeolitic imidazolate framework followed by thermal activation. The catalyst offers a carbon nanonetwork architecture made of microporous nanofibers decorated by uniformly distributed high-density active sites. In a single-cell test, the membrane electrode containing such a catalyst delivered unprecedented volumetric activities of 3.3 A⋅cm−3 at 0.9 V or 450 A⋅cm−3 extrapolated at 0.8 V, representing the highest reported value in the literature. Improved fuel cell durability was also observed. PMID:26261338

  13. 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.

  14. 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 interaction between perfluorosulfonic acid ionomer and supported platinum catalyst is essential. It directly influences platinum accessibility, stability of carbon support and platinum, proton conductivity and electron conductivity in an electrode. In this study, we compare the adsorption...... that the platinization step modifies the surface nature of the carbon supports in terms of specific surface area, crystallinity and especially porosity; therefore, ionomer adsorption over carbon is not always representative for the ionomer adsorption over carbon supported catalyst, though indicative. Moreover...

  15. Synthesis of vertical MnO2 wire arrays on hemp-derived carbon for efficient and robust green catalysts

    Science.gov (United States)

    Yang, MinHo; Kim, Dong Seok; Sim, Jae-Wook; Jeong, Jae-Min; Kim, Do Hyun; Choi, Jae Hyung; Kim, Jinsoo; Kim, Seung-Soo; Choi, Bong Gill

    2017-06-01

    Three-dimensional (3D) carbon materials derived from waste biomass have been attracted increasing attention in catalysis and materials science because of their great potential of catalyst supports with respect to multi-functionality, unique structures, high surface area, and low cost. Here, we present a facile and efficient way for preparing 3D heterogeneous catalysts based on vertical MnO2 wires deposited on hemp-derived 3D porous carbon. The 3D porous carbon materials are fabricated by carbonization and activation processes using hemp (Cannabis Sttiva L.). These 3D porous carbon materials are employed as catalyst supports for direct deposition of vertical MnO2 wires using a one-step hydrothermal method. The XRD and XPS results reveal the crystalline structure of α-MnO2 wires. The resultant composites are further employed as a catalyst for glycolysis of poly(ethylene terephthalate) (PET) with high conversion yield of 98%, which is expected to be expressly profitable for plastics recycling industry.

  16. Synthesis and characterization of nanometal-ordered mesoporous carbon composites as heterogeneous catalysts for electrooxidation of aniline

    International Nuclear Information System (INIS)

    Duan, Xiaoyue; Chen, Yawen; Liu, Xinyue; Chang, Limin

    2017-01-01

    Highlights: •NM-OMC catalysts were prepared for electrochemical oxidation of aniline. •The oxidation of aniline was studied with NM-OMC catalysts suspended in solution. •The Cu-OMC exhibited the highest catalytic activity for aniline degradation. •The mineralization current efficiency was improved by 2 times with Cu-OMC catalyst. •An electrochemical mineralization pathway of aniline was proposed. -- Abstract: The Cu, Co and Ni nanometal embedded ordered mesoporous carbons (NM-OMCs) were fabricated by a soft-template method using phenol/formaldehyde as carbon source and triblock copolymer F127 as template agent. The morphology, structure, surface physicochemical properties and pore structure of the NM-OMCs were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscope (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and nitrogen adsorption-desorption isotherms. Their potential application to the electrocatalytic degradation of aniline was investigated using electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and ·OH radicals generation test. Furthermore, the electrochemical oxidation process of aniline was also investigated in the presence of the OMC-based catalyst particles suspended in a Na 2 SO 4 solution using a PbO 2 anode. Results revealed that the NM-OMCs inherited the ordered mesostructure of pristine OMC and the metal nanoparticles (Cu, Co or Ni) were embedded in the carbon framework. The Cu-OMC exhibited significantly higher catalytic activity than OMC and other NM-OMCs for the electrooxidation of aniline. In electrochemical oxidation process of aniline, nearly all of aniline could be degraded after 120 min of electrolysis with Cu-OMC particles as catalyst, while 89%, 92%, and 97% with OMC, Co-OMC and Ni-OMC catalysts, respectively, obviously higher than 76% of electrochemical oxidation without assistance of catalysts. After

  17. 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

  18. New Method to Synthesize Highly Active and Durable Chemically Ordered fct-PtCo Cathode Catalyst for PEMFCs.

    Science.gov (United States)

    Jung, Won Suk; Popov, Branko N

    2017-07-19

    In the bottom-up synthesis strategy performed in this study, the Co-catalyzed pyrolysis of chelate-complex and activated carbon black at high temperatures triggers the graphitization reaction which introduces Co particles in the N-doped graphitic carbon matrix and immobilizes N-modified active sites for the oxygen reduction reaction (ORR) on the carbon surface. In this study, the Co particles encapsulated within the N-doped graphitic carbon shell diffuse up to the Pt surface under the polymer protective layer and forms a chemically ordered face-centered tetragonal (fct) Pt-Co catalyst PtCo/CCCS catalyst as evidenced by structural and compositional studies. The fct-structured PtCo/CCCS at low-Pt loading (0.1 mg Pt cm -2 ) shows 6% higher power density than that of the state-of-the-art commercial Pt/C catalyst. After the MEA durability test of 30 000 potential cycles, the performance loss of the catalyst is negligible. The electrochemical surface area loss is less than 40%, while that of commercial Pt/C is nearly 80%. After the accelerated stress test, the uniform catalyst distribution is retained and the mean particle size increases approximate 1 nm. The results obtained in this study indicated that highly stable compositional and structural properties of chemically ordered PtCo/CCCS catalyst contribute to its exceptional catalyst durability.

  19. Ferromagnetic resonance of cobalt nanoparticles used as a catalyst for the carbon nanotubes synthesis

    Energy Technology Data Exchange (ETDEWEB)

    Duraia, El-Shazly M. [Suez Canal University, Faculty of Science, Physics Department, Ismailia (Egypt); Al-Farabi Kazakh National University, Almaty (Kazakhstan); Institute of Physics and Technology, Almaty (Kazakhstan)], E-mail: duraia_physics@yahoo.com; Abdullin, Kh.A. [Institute of Physics and Technology, Almaty (Kazakhstan)

    2009-12-15

    Catalyst is considered to be the most crucial parameter for the growth of carbon nanotubes. In this work we study the ferromagnetic resonance (FMR) spectra of the catalyst nanoclusters. Moreover we report for the first time the angle FMR studies of catalyst particles with and without CNT layer. The dependencies of the FMR spectra, X-ray diffraction (XRD) patterns, Raman spectra and morphology of the CNT layers on the growth conditions are discussed.

  20. Influence of Synthesis pH on Textural Properties of Carbon Xerogels as Supports for Pt/CXs Catalysts for Direct Methanol Fuel Cells

    Directory of Open Access Journals (Sweden)

    C. Alegre

    2012-01-01

    Full Text Available Carbon xerogels (CXs have been prepared by polycondensation of resorcinol and formaldehyde. Two synthesis pHs were studied in order to evaluate its influence on the electrochemical behaviour of Pt catalysts supported on previous carbon xerogels, synthesized by conventional impregnation method. Catalysts were also synthesized over a commercial carbon black (Vulcan-XC-72R for comparison purposes. Characterization techniques included nitrogen physisorption, scanning electron microscopy, and X-ray diffraction. Catalysts electrochemical activity towards the oxidation of carbon monoxide and methanol was studied by cyclic voltammetry and chronoamperometry to establish the effect of the carbon support on the catalysts performance. Commercial Pt/C catalyst (E-TEK was analyzed for comparison purposes. It was observed that the more developed and mesopore-enriched porous structure of the carbon xerogel synthesized at a higher initial pH resulted in an optimal utilization of the active phase and in an enhanced and promising catalytic activity in the electrooxidation of methanol, in comparison with commercial catalysts.

  1. Catalytic activity of zeolite-containing catalysts in cumene cracking

    Energy Technology Data Exchange (ETDEWEB)

    Koval' chuk, L V; Takhtarova, G N; Topchieva, K V [Moskovskij Gosudarstvennyj Univ. (USSR). Kafedra Fizicheskoj Khimii

    1977-01-01

    The catalytic properties are studied of decationized forms (Ca and La) of zeolite-containing catalysts in relation to the nature of the cation and the degree of exchange in the cumene cracking reaction. It has been established that the increase in the activity of Ca-decationized catalysts occurs at a degree of exchange from 22 to 40% and at a ratio of the cation and decationized areas from 0.4 to 1. For La-decationized catalysts the activity increases at a degree of exchange up to 60% and at a ratio between the cation and decationized areas exceeding 1.

  2. Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Hanguang [Department; Hwang, Sooyeon [Center; Wang, Maoyu [School; Feng, Zhenxing [School; Karakalos, Stavros [Department; Luo, Langli [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Qiao, Zhi [Department; Xie, Xiaohong [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Wang, Chongmin [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Su, Dong [Center; Shao, Yuyan [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Wu, Gang [Department

    2017-09-26

    To significantly reduce the cost of proton exchange membrane (PEM) fuel cells, current Pt must be replaced by platinum-metal-group (PGM)-free catalysts for the oxygen reduction reaction (ORR) in acid. We report here a new class of high-performance atomic iron dispersed carbon catalysts through controlled chemical doping of iron ions into zinc-zeolitic imidazolate framework (ZIF), a type of metal-organic framework (MOF). The novel synthetic chemistry enables accurate size control of Fe-doped ZIF catalyst particles with a wide range from 20 to 1000 nm without changing chemical properties, which provides a great opportunity to increase the density of active sites that is determined by the particle size. We elucidated the active site formation mechanism by correlating the chemical and structural changes with thermal activation process for the conversion from Fe-N4 complex containing hydrocarbon networks in ZIF to highly active FeNx sites embedded into carbon. A temperature of 800oC was identified as the critical point to start forming pyridinic nitrogen doping at the edge of the graphitized carbon planes. Further increasing heating temperature to 1100oC leads to increase of graphitic nitrogen, generating possible synergistic effect with FeNx sites to promote ORR activity. The best performing catalyst, which has well-defined particle size around 50 nm and abundance of atomic FeNx sites embedded into carbon structures, achieve a new performance milestone for the ORR in acid including a half-wave potential of 0.85 V vs RHE and only 20 mV loss after 10,000 cycles in O2 saturated H2SO4 electrolyte. The new class PGM-free catalyst with approaching activity to Pt holds great promise for future PEM fuel cells.

  3. A smart strategy to fabricate Ru nanoparticle inserted porous carbon nanofibers as highly efficient levulinic acid hydrogenation catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Ying; Sun, Cheng-Jun; Brown, Dennis E.; Zhang, Liqiang; Yang, Feng; Zhao, Hairui; Wang, Yue; Ma, Xiaohui; Zhang, Xin; Ren, Yang

    2016-01-01

    Herein, we first put forward a smart strategy to in situ fabricate Ru nanoparticle (NP) inserted porous carbon nanofibers by one-pot conversion of Ru-functionalized metal organic framework fibers. Such fiber precursors are skillfully constructed by cooperative assembly of different proportional RuCl3 and Zn(Ac)2·2H2O along with trimesic acid (H3BTC) in the presence of N,N-dimethylformamide. The following high-temperature pyrolysis affords uniform and evenly dispersed Ru NPs (ca. 12-16 nm), which are firmly inserted into the hierarchically porous carbon nanofibers formed simultaneously. The resulting Ru-carbon nanofiber (Ru-CNF) catalysts prove to be active towards the liquid-phase hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL), a biomass-derived platform molecule with wide applications in the preparation of renewable chemicals and liquid transportation fuels. The optimal GVL yield of 96.0% is obtained, corresponding to a high activity of 9.23 molLAh–1gRu–1, 17 times of that using the commercial Ru/C catalyst. Moreover, the Ru-CNF catalyst is extremely stable, and can be cycled up to 7 times without significant loss of reactivity. Our strategy demonstrated here reveals new possibilities to make proficient metal catalysts, and provides a general way to fabricate metal-carbon nanofiber composites available for other applications.

  4. Characterizing the structural degradation in a PEMFC cathode catalyst layer : carbon corrosion

    Energy Technology Data Exchange (ETDEWEB)

    Young, A.; Stumper, J. [Ballard Power Systems, Burnaby, BC (Canada); Gyenge, E. [British Columbia Univ., Vancouver, BC (Canada). Dept. of Chemical and Biological Engineering

    2009-07-01

    The structural degradation resulting from carbon corrosion of a cathode catalyst layer in a polymer electrolyte membrane fuel cell (PEMFC) was investigated in this study. In order to oxidize the catalyst carbon support, the PEMFC catalyst layer was subjected to a 30 hour accelerated stress test that cycled the cathode potential from 0.1 to 1.5 VRHE at 30 and 150 second intervals. The rate and amount of carbon loss was determined by measuring the carbon dioxide in the exhaust gas. The structural degradation of the catalyst layer was characterized and correlated to the PEMFC performance using cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM) and polarization analyses. This analysis revealed a clear thinning of the cathode catalyst layer and gas diffusion layer carbon sub-layer, and a reduction in the effective platinum surface area due to the carbon support oxidation. The thinned cathode catalyst layer changed the water management, and increased the voltage loss associated with the oxygen mass transport and catalyst layer ohmic resistance. In order to further develop and verify this methodology for other degradation mechanisms, emphasis was placed on EIS measurements.

  5. Metal-phthalocyanine functionalized carbon nanotubes as catalyst for the oxygen reduction reaction: A theoretical study

    Science.gov (United States)

    Orellana, Walter

    2012-07-01

    The covalent functionalization of metallic single-walled carbon nanotubes (CNTs) with transition metal phthalocyanines (MPc, with M = Mn, Fe and Co) are addressed by density functional calculations. The CNT-MPc catalytic activity toward the oxygen reduction reaction (ORR) is investigated through the O2 stretching frequency adsorbed on the phthalocyanine metal center. We find better reduction abilities when the CNT functionalization occurs through sp2-like bonds. Multiple stable-spin states for the M-O2 adduct are also found for M = Mn and Fe, suggesting higher ORR rates. The CNT-MPc complexes show metallic characteristics, suggesting favorable conditions to work as ORR cathode catalysts in fuel cells.

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

    Science.gov (United States)

    Mirabile Gattia, Daniele; Antisari, Marco Vittori; Giorgi, Leonardo; Marazzi, Renzo; Piscopiello, Emanuela; Montone, Amelia; Bellitto, Serafina; Licoccia, Silvia; Traversa, Enrico

    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.

  7. Activated carbon supported CaO for conversion of palm oil to ...

    African Journals Online (AJOL)

    In this study, activated carbon supported CaO catalyst was used for the transesterification reaction of palm oil. The catalyst was prepared according to the conventional incipient witness impregnation method. Kinetic experiment was performed in a batch reactor in the presence of heterogeneous catalyst for a wide range of ...

  8. Influence of Chemical and Physical Properties of Activated Carbon Powders on Oxygen Reduction and Microbial Fuel Cell Performance

    KAUST Repository

    Watson, Valerie J.; Nieto Delgado, Cesar; Logan, Bruce E.

    2013-01-01

    Commercially available activated carbon (AC) powders made from different precursor materials (coal, peat, coconut shell, hardwood, and phenolic resin) were electrochemically evaluated as oxygen reduction catalysts and tested as cathode catalysts

  9. 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.

  10. Design of Polymer-Coated Multi-Walled Carbon Nanotube/Carbon Black-based Fuel Cell Catalysts with High Durability and Performance Under Non-humidified Condition

    International Nuclear Information System (INIS)

    Yang, Zehui; Berber, Mohamed R.; Nakashima, Naotoshi

    2015-01-01

    To realize a high catalyst utilization, better fuel cell performance and durability as well as low production cost, an efficient design strategy of the catalyst layer that can improve both the oxygen accessibility and structure stability is highly required. Here, we describe the preparation of fuel cell electrocatalysts with an efficient fuel cell performance and better stability based on hybrids of multi-walled carbon nanotubes (MWNTs) and carbon black (CB) which were wrapped by a proton conducting polymer, poly[2,2′-(2,6-pyridine)-5,5′-bibenzimidazole], before deposition of the platinum (Pt) metal catalyst. The catalyst mass activity after feeding only 10%-MWNTs to CB increased by 1.5 and 2 times than those of the MWNTs-based- and CB-based catalysts, respectively. The results also demonstrated that 90 wt% of the MWNTs in the catalyst layer allows it to be replaced by CB without any significant change in its durability and performance under 120 °C and non-humidified condition

  11. 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.

  12. Influence of surface morphology on methanol oxidation at a glassy carbon-supported Pt catalyst

    Directory of Open Access Journals (Sweden)

    S. STEVANOVIC

    2008-08-01

    Full Text Available Platinum supported on glassy carbon (GC was used as a model system for studying the influence of the surface morphology of a Pt catalyst on methanol oxidation in alkaline and acidic solutions. Platinum was deposited by the potential step method on GC samples from H2SO4 + H2PtCl6 solution under the same conditions with loadings from 10 to 80 mg cm-2. AFM and STM images of the GC/Pt electrodes showed that the Pt was deposited in the form of 3D agglomerates composed of spherical particles. Longer deposition times resulted in increased growth of Pt forms and a decrease in the specific area of the Pt. The real surface area of Pt increased with loading but the changes were almost negligible at higher loadings. Nevertheless, both the specific and mass activity of platinum supported on glassy carbon for methanol oxidation in acidic and in alkaline solutions exhibit a volcanic dependence with respect to the platinum loading. The increase in the activity can be explained by the increasing the particle size with the loading and thus an increase in the contiguous Pt sites available for adsorption and decomposition of methanol. However, the decrease in the activity of the catalyst with further increase of loading and particle size after reaching the maximum is related to the decrease of active sites available for methanol adsorption and their accessibility as a result of more close proximity and pronounced coalescence of the Pt particles.

  13. 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...... of the dopant alkali compounds varied from 1 to 5%. As prepared CNTs were characterized by transmission electron microscopy (TEM), X‐ray diffraction (XRD) and Raman microscopy. Results revealed that both carbon yield and deposit could be increased over doped catalysts.......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...

  14. Activated carbon material

    International Nuclear Information System (INIS)

    Evans, A.G.

    1978-01-01

    Activated carbon particles for use as iodine trapping material are impregnated with a mixture of selected iodine and potassium compounds to improve the iodine retention properties of the carbon. The I/K ratio is maintained at less than about 1 and the pH is maintained at above about 8.0. The iodine retention of activated carbon previously treated with or coimpregnated with triethylenediamine can also be improved by this technique. Suitable flame retardants can be added to raise the ignition temperature of the carbon to acceptable standards

  15. Effect of heat treatment on stability of gold particle modified carbon supported Pt-Ru anode catalysts for a direct methanol fuel cell

    International Nuclear Information System (INIS)

    Li Xiaowei; Liu Juanying; Huang Qinghong; Vogel, Walter; Akins, Daniel L.; Yang Hui

    2010-01-01

    Carbon supported Au-PtRu (Au-PtRu/C) catalysts were prepared as the anodic catalysts for the direct methanol fuel cell (DMFC). The procedure involved simple deposition of Au particles on a commercial Pt-Ru/C catalyst, followed by heat treatment of the resultant composite catalyst at 125, 175 and 200 o C in a N 2 atmosphere. High-resolution transmission electron microscopy (HR-TEM) measurements indicated that the Au nanoparticles were attached to the surface of the Pt-Ru nanoparticles. We found that the electrocatalytic activity and stability of the Au-PtRu/C catalysts for methanol oxidation is better than that of the PtRu/C catalyst. An enhanced stability of the electrocatalyst is observed and attributable to the promotion of CO oxidation by the Au nanoparticles adsorbed onto the Pt-Ru particles, by weakening the adsorption of CO, which can strongly adsorb to and poison Pt catalyst. XPS results show that Au-PtRu/C catalysts with heat treatment lead to surface segregation of Pt metal and an increase in the oxidation state of Ru, which militates against the dissolution of Ru. We additionally find that Au-PtRu/C catalysts heat-treated at 175 o C exhibit the highest electrocatalytic stability among the catalysts prepared by heat treatment: this observation is explained as due to the attainment of the highest relative concentration of gold and the highest oxidation state of Ru oxides for the catalyst pretreated at this temperature.

  16. Fabrication of Fischer-Tropsch Catalysts by Deposition of Iron Nanocrystals on Carbon Nanotubes

    NARCIS (Netherlands)

    Casavola, Marianna; Hermannsdoerfer, Justus; de Jonge, Niels; Dugulan, A. Iulian; de Jong, Krijn P.

    2015-01-01

    The fabrication of supported catalysts consisting of colloidal iron oxide nanocrystals with tunable size, geometry, and loadinghomogeneously dispersed on carbon nanotube (CNT) supportsis described herein. The catalyst synthesis is performed in a two-step approach. First, colloidal iron and iron

  17. 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

  18. 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

  19. 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.

  20. Influence of the catalyst type on the growth of carbon nanotubes via methane chemical vapor deposition

    NARCIS (Netherlands)

    Jodin, Lucie; Dupuis, Anne-Claire; Rouvière, Emmanuelle; Reiss, Peter

    2006-01-01

    The preparation of the catalyst is one of the key parameters which governs the quality of carbon nanotubes (CNTs) grown by catalyzed chemical vapor deposition (CVD). We investigated the influence of three different procedures of catalyst preparation on the type and diameter of CNTs formed under

  1. 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.

  2. High-performance bimetallic alloy catalyst using Ni and N co-doped composite carbon for the oxygen electro-reduction.

    Science.gov (United States)

    Jung, Won Suk

    2018-03-15

    In this study, a novel synthesis method for the bimetallic alloy catalyst is reported, which is subsequently used as an oxygen reduction catalyst in polymer electrolyte membrane fuel cells (PEMFCs). The support prepared from the Ni-chelate complex shows a mesoporous structure with a specific surface area of ca. 400 m 2  g -1 indicating the suitable support for PEMFC applications. Ethylenediamine is converted to the nitrogen and carbon layers to protect the Ni particles which will diffuse into the Pt lattice at 800 °C. The PtNi/NCC catalyst with PtNi cores and Pt-rich shells is successfully formed when acid-treated as evidenced by line scan profiles. The catalyst particles thus synthesized are well-dispersed on the N-doped carbon support, while the average particle size is ca. 3 nm. In the PEMFC test, the maximum power density of the PtNi/NCC catalyst shows approximately 25% higher than that of the commercial Pt/C catalyst. The mass activity of the PtNi/NCC catalyst showed approximately 3-fold higher than that of the commercial Pt/C catalyst. The mass activity strongly depends on the ratio of Pt to Ni since the strain effect can be strong for catalysts due to the mismatch of lattice parameters of the Ni and Pt. Copyright © 2017 Elsevier Inc. All rights reserved.

  3. Carbon monoxide oxidation over three different states of copper: Development of a model metal oxide catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Jernigan, Glenn Geoffrey [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 (Cu2O), 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 > Cu2O > CuO) and the activation energy increased with increasing oxidation state (Cu, 9 kcal/mol < Cu2O, 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 N2 and CO2. At the end of each reaction, the catalyst was found to be Cu2O. There is a need to study the kinetics of this reaction over the different oxidation states of copper.

  4. Influence of metal coating methods on the activity of bimetal-containing zeolite catalysts of Co, Pd-ZSM-5 in carbon monoxide oxidation

    Science.gov (United States)

    Oleksenko, L. P.; Lutsenko, L. V.; Yatsimirskii, V. K.

    2011-07-01

    It has been established that catalytic activity in the CO oxidation of bimetal-containing zeolite Co,Pd-systems based on ZSM-5 and obtained via ion exchange and impregnation at different orders of the introduction of metal cations is higher than that of monometal-containing systems Co-ZSM-5 and Pd—ZSM-5. Through TPD of NH3, it was determined that coordination-unsaturated bicationic associates are formed in Co,Pd/ZSM-5 zeolites obtained by ion exchange. It was found that the activity of bimetal-containing systems depends on the relation of the active components.

  5. 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.

  6. Nitrogen-Doped Carbon Encapsulated Nickel/Cobalt Nanoparticle Catalysts for Olefin Migration of Allylarenes

    DEFF Research Database (Denmark)

    Kramer, Søren; Mielby, Jerrik Jørgen; Buss, Kasper Spanggård

    2017-01-01

    Olefin migration of allylarenes is typically performed with precious metal-based homogeneous catalysts. In contrast, very limited progress has been made using cheap, earth-abundant base metals as heterogeneous catalysts for these transformations - in spite of the obvious economic and environmental...... advantages. Herein, we report on the use of an easily prepared heterogeneous catalyst material for the migration of olefins, in particular allylarenes. The catalyst material consists of nickel/cobalt alloy nanoparticles encapsulated in nitrogen-doped carbon shells. The encapsulated nanoparticles are stable...

  7. Metal-free carbon materials-catalyzed sulfate radical-based advanced oxidation processes: A review on heterogeneous catalysts and applications.

    Science.gov (United States)

    Zhao, Qingxia; Mao, Qiming; Zhou, Yaoyu; Wei, Jianhong; Liu, Xiaocheng; Yang, Junying; Luo, Lin; Zhang, Jiachao; Chen, Hong; Chen, Hongbo; Tang, Lin

    2017-12-01

    In recent years, advanced oxidation processes (AOPs), especially sulfate radical based AOPs have been widely used in various fields of wastewater treatment due to their capability and adaptability in decontamination. Recently, metal-free carbon materials catalysts in sulfate radical production has been more and more concerned because these materials have been demonstrated to be promising alternatives to conventional metal-based catalysts, but the review of metal-free catalysts is rare. The present review outlines the current state of knowledge on the generation of sulfate radical using metal-free catalysts including carbon nanotubes, graphene, mesoporous carbon, activated carbon, activated carbon fiber, nanodiamond. The mechanism such as the radical pathway and non-radical pathway, and factors influencing of the activation of sulfate radical was also be revealed. Knowledge gaps and research needs have been identified, which include the perspectives on challenges related to metal-free catalyst, heterogeneous metal-free catalyst/persulfate systems and their potential in practical environmental remediation. Copyright © 2017 Elsevier Ltd. All rights reserved.

  8. Study of the catalytic activity of supported technetium catalysts

    International Nuclear Information System (INIS)

    Spitsyn, V.I.; Mikhailenko, I.E.; Pokorovskaya, O.V.

    1985-01-01

    The radioactive d metal 43 Tc 99 has catalytic properties in the synthesis of ammonia. For the purpose of reducing the quantity of the radioactive metal and of increasing the specific surface, the active component was applied to BaTiO 3 and gamma-Al 2 O 3 supports. This paper uses charcoal as a support and a table presents the catalytic activity of the samples during the synthesis of ammonia. X-ray diffractometric investigation of the catalysts was carried out with the use of Cu K /SUB alpha/ radiation. It is shown that the catalysts. The values of the specific rate constants of technetium in the catalysts. The values of the specific rate constants remain practically constant for all the catalyst samples studied, attesting to the absence of a specific metal-support interaction during the synthesis of ammonia

  9. Energy storage applications of activated carbons: supercapacitors and hydrogen storage

    OpenAIRE

    Sevilla Solís, Marta; Mokaya, Robert

    2014-01-01

    Porous carbons have several advantageous properties with respect to their use in energy applications that require constrained space such as in electrode materials for supercapacitors and as solid state hydrogen stores. The attractive properties of porous carbons include, ready abundance, chemical and thermal stability, ease of processability and low framework density. Activated carbons, which are perhaps the most explored class of porous carbons, have been traditionally employed as catalyst s...

  10. Petroleum residue upgrading with dispersed catalysts. Part 1. Catalysts activity and selectivity

    Energy Technology Data Exchange (ETDEWEB)

    Panariti, N.; Del Bianco, A.; Del Piero, G. [ENITECNOLOGIE S.p.A, Via Maritano 26, 20097 San Donato Mil. (Italy); Marchionna, M. [SNAMPROGETTI S.p.A, Via Maritano 26, 20097 San Donato Mil. (Italy)

    2000-12-04

    The results of a study aimed at the identification of the relevant chemical aspects involved in the process of upgrading heavy feedstocks in the presence of dispersed catalysts are discussed. The catalytic activity of different compounds was compared in terms of products yields and quality. Moreover, a detailed and systematic characterization of the catalysts recovered at the end of the reactions was achieved. The experimental work provided quite a large set of data, allowing to investigate the factors that may affect catalyst activity (precursor solubility, rate of activation, degree of dispersion, presence of promoters, etc.). The results of this study demonstrate that the best performances are obtained by the microcrystalline molybdenite generated in situ by oil-soluble precursors. The nature of the organic ligand does not play a very relevant role in influencing the hydrogenation activity. The presence of phosphorus, however, significantly enhances hydrodemetallation, at least in terms of vanadium removal. Bimetallic precursors show a slight synergistic effect towards the hydrodesulfurization reaction. Microsized powdered catalyst precursors have a much lower catalytic activity compared to the oil-soluble ones.

  11. Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Hanguang; Hwang, Sooyeon; Wang, Maoyu; Feng, Zhenxing; Karakalos, Stavros; Luo, Langli; Qiao, Zhi; Xie, Xiaohong; Wang, Chongmin; Su, Dong; Shao, Yuyan; Wu, Gang (BNL); (Oregon State U.); (SC); (PNNL); (Buffalo)

    2017-09-26

    It remains a grand challenge to replace platinum group metal (PGM) catalysts with earth-abundant materials for the oxygen reduction reaction (ORR) in acidic media, which is crucial for large-scale deployment of proton exchange membrane fuel cells (PEMFCs). Here, we report a high-performance atomic Fe catalyst derived from chemically Fe-doped zeolitic imidazolate frameworks (ZIFs) by directly bonding Fe ions to imidazolate ligands within 3D frameworks. Although the ZIF was identified as a promising precursor, the new synthetic chemistry enables the creation of well-dispersed atomic Fe sites embedded into porous carbon without the formation of aggregates. The size of catalyst particles is tunable through synthesizing Fe-doped ZIF nanocrystal precursors in a wide range from 20 to 1000 nm followed by one-step thermal activation. Similar to Pt nanoparticles, the unique size control without altering chemical properties afforded by this approach is able to increase the number of PGM-free active sites. The best ORR activity is measured with the catalyst at a size of 50 nm. Further size reduction to 20 nm leads to significant particle agglomeration, thus decreasing the activity. Using the homogeneous atomic Fe model catalysts, we elucidated the active site formation process through correlating measured ORR activity with the change of chemical bonds in precursors during thermal activation up to 1100 °C. The critical temperature to form active sites is 800 °C, which is associated with a new Fe species with a reduced oxidation number (from Fe3+ to Fe2+) likely bonded with pyridinic N (FeN4) embedded into the carbon planes. Further increasing the temperature leads to continuously enhanced activity, linked to the rise of graphitic N and Fe–N species. The new atomic Fe catalyst has achieved respectable ORR activity in challenging acidic media (0.5 M H2SO4), showing a half-wave potential of 0.85 V vs RHE and leaving only a 30 mV gap with Pt/C (60 μgPt/cm2). Enhanced stability

  12. Selective deposition of catalyst nanoparticles using the gravitational force for carbon nanotubes interconnect

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Do-Yoon; Lee, Hyun-Chul; Lee, Jong-Hak; Park, Jae-Hong; Alegaonkar, Prashant S. [Center for Nanotubes and Nanostructured Composites, Sungkyunkwan University, 300 Chunchun-dong, Jangan-Gu, Suwon, 440-746 (Korea, Republic of); Yoo, Ji-Beom [Center for Nanotubes and Nanostructured Composites, Sungkyunkwan University, 300 Chunchun-dong, Jangan-Gu, Suwon, 440-746 (Korea, Republic of)], E-mail: jbyoo@skku.ac.kr; Han, In-Taek; Kim, Ha-Jin; Jin, Yong-Wan; Kim, Jong-Min [Samsung Advanced Institute of Technology, Mt. 14-1, Nongseo-dong, Giheung-gu, Younggin-si Gyunggi-do, 449-712 (Korea, Republic of); Kwon, Kee-Won [Department of Semiconducting System, Sungkyunkwan University (Korea, Republic of)

    2008-04-01

    The photolithography process has generally been used for the making of catalyst layers used for the synthesis of CNTs due to its comparative ease. However, this method results in the formation of undesirable catalyst particles, which deteriorate the quality of the devices. Therefore, we tried to form a catalyst layer without using any lift-off or wet etching process, especially for the formation of carbon nanotube interconnects. After spin coating the samples, which were previously fabricated with several vias, with an iron-acetate solution, the catalyst layer was pulled down into the bottom of the holes through the force of gravity. We were able to remove the catalyst layer which was coated over undesirable areas, by TMAH (tetramethylammonium hydroxide, N(CH{sub 3}){sub 4}OH) treatment. After the catalyst deposition process, we synthesized CNTs and observed them by scanning electron microscopy (SEM)

  13. Carbon-Supported Pd and PdFe Alloy Catalysts for Direct Methanol Fuel Cell Cathodes

    Directory of Open Access Journals (Sweden)

    Luis M. Rivera Gavidia

    2017-05-01

    Full Text Available Direct methanol fuel cells (DMFCs are electrochemical devices that efficiently produce electricity and are characterized by a large flexibility for portable applications and high energy density. Methanol crossover is one of the main obstacles for DMFC commercialization, forcing the search for highly electro-active and methanol tolerant cathodes. In the present work, carbon-supported Pd and PdFe catalysts were synthesized using a sodium borohydride reduction method and physico-chemically characterized using transmission electron microscopy (TEM and X-ray techniques such as photoelectron spectroscopy (XPS, diffraction (XRD and energy dispersive spectroscopy (EDX. The catalysts were investigated as DMFC cathodes operating at different methanol concentrations (up to 10 M and temperatures (60 °C and 90 °C. The cell based on PdFe/C cathode presented the best performance, achieving a maximum power density of 37.5 mW·cm−2 at 90 °C with 10 M methanol, higher than supported Pd and Pt commercial catalysts, demonstrating that Fe addition yields structural changes to Pd crystal lattice that reduce the crossover effects in DMFC operation.

  14. 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.

  15. A "catalyst switch" Strategy for the sequential metal-free polymerization of epoxides and cyclic Esters/Carbonate

    KAUST Repository

    Zhao, Junpeng; Pahovnik, David; Gnanou, Yves; Hadjichristidis, Nikolaos

    2014-01-01

    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.

  16. Recent development of active nanoparticle catalysts for fuel cell reactions

    Energy Technology Data Exchange (ETDEWEB)

    Mazumder, Vismadeb; Lee, Youngmin; Sun, Shouheng [Department of Chemistry Brown University Providence, RI (United States)

    2010-04-23

    This review focuses on the recent advances in the synthesis of nanoparticle (NP) catalysts of Pt-, Pd- and Au-based NPs as well as composite NPs. First, new developments in the synthesis of single-component Pt, Pd and Au NPs are summarized. Then the chemistry used to make alloy and composite NP catalysts aiming to enhance their activity and durability for fuel cell reactions is outlined. The review next introduces the exciting new research push in developing CoN/C and FeN/C as non-Pt catalysts. Examples of size-, shape- and composition-dependent catalyses for oxygen reduction at cathode and formic acid oxidation at anode are highlighted to illustrate the potentials of the newly developed NP catalysts for fuel cell applications. (Abstract Copyright [2010], Wiley Periodicals, Inc.)

  17. Support effects on hydrotreating activity of NiMo catalysts

    International Nuclear Information System (INIS)

    Dominguez-Crespo, M.A.; Arce-Estrada, E.M.; Torres-Huerta, A.M.; Diaz-Garcia, L.; Cortez de la Paz, M.T.

    2007-01-01

    The effect of the gamma alumina particle size on the catalytic activity of NiMoS x catalysts prepared by precipitation method of aluminum acetate at pH = 10 was studied. The structural characterization of the supports was measured by using XRD, pyridine FTIR-TPD and nitrogen physisorption. NiMo catalysts were characterized during the preparation steps (annealing and sulfidation) using transmission electron microscopy (TEM). Hydrogen TPR studies of the NiMo catalysts were also carried out in order to correlate their hydrogenating properties and their catalytic functionality. Catalytic tests were carried out in a pilot plant at 613, 633 and 653 K temperatures. The results showed that the rate constants of hydrodesulfurization (HDS), hydrodenitrogenation (HDN) and hydrodearomatizing (HDA) at 613-653 K decreased in the following order: A > B > C corresponding to the increase of NiMoS particle size associated to these catalysts

  18. 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.

  19. More active and sulfur resistant bimetallic Pd-Ni catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Betti, Carolina; Carrara, Nicolás; Badano, Juan; Lederhos, Cecilia; Vera, Carlos; Quiroga, Mónica, E-mail: mquiroga@fiq.unl.edu.ar [Instituto de Investigaciones en Catálisis y Petroquímica, INCAPE (FIQ-UNL, CONICET), Santa Fe (Argentina)

    2018-02-15

    The influence of the kind of metal precursor and the sequence of impregnation on the properties of Pd-Ni catalysts was evaluated during the test reaction of selective hydrogenation of styrene to ethylbenzene by means of physicochemical characterization. The focus was put on the final hydrogenating activity and the resistance to deactivation by sulfide compounds (thiophene). The used techniques of characterization were ICP, XPS, XDR, TPR, CO chemisorption and TEM. XPS results indicated the presence of different Pd species: Pd{sup δ-}, Pd{sup 0} and Pd{sup δ+}. In the case of the Ni containing catalysts, Ni{sup 0} and NiO species were also detected. These palladium and nickel species would be responsible of the variation of activity and sulfur resistance of the catalysts. NiClPd catalysts had a higher resistance to deactivation by sulfur poisoning. This was associated to a higher concentration of Pd{sup η+}Cl{sub x}O{sub y} species that would prevent the adsorption of thiophene by both steric and electronic effects. It could also be due to the lower concentration of Pd{sup 0} and Ni{sup 0} on these catalysts, as compared to those shown by the PdNiCl catalysts. Both the Pd{sup 0} and Ni{sup 0} species are more prone to poisoning because of their higher electronic availability. (author)

  20. 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.

  1. 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

  2. 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.

  3. Flame synthesis of carbon nano onions using liquefied petroleum gas without catalyst

    International Nuclear Information System (INIS)

    Dhand, Vivek; Prasad, J. Sarada; Rao, M. Venkateswara; Bharadwaj, S.; Anjaneyulu, Y.; Jain, Pawan Kumar

    2013-01-01

    Densely agglomerated, high specific surface area carbon nano onions with diameter of 30–40 nm have been synthesized. Liquefied petroleum gas and air mixtures produced carbon nano onions in diffusion flames without catalyst. The optimized oxidant to fuel ratio which produces carbon nano onions has been found to be 0.1 slpm/slpm. The experiment yielded 70% pure carbon nano onions with a rate of 5 g/h. X-ray diffraction, high-resolution electron microscopy and Raman spectrum reveal the densely packed sp 2 hybridized carbon with (002) semi-crystalline hexagonal graphite reflection. The carbon nano onions are thermally stable up to 600 °C. - Highlights: ►Flame synthesized carbon nano onions with 30–40 nm diameters. ►LPG/air, diffusion type flame used in absence of catalyst to produce nano onions. ►Carbon nano onion production rate is 5 g/hr and with 70% purity.

  4. 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)

    Shuit, Siew Hoong; Tan, Soon Huat

    2014-01-01

    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. • SO 3 H 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

  5. Toward Small-Diameter Carbon Nanotubes Synthesized from Captured Carbon Dioxide: Critical Role of Catalyst Coarsening.

    Science.gov (United States)

    Douglas, Anna; Carter, Rachel; Li, Mengya; Pint, Cary L

    2018-05-23

    Small-diameter carbon nanotubes (CNTs) often require increased sophistication and control in synthesis processes, but exhibit improved physical properties and greater economic value over their larger-diameter counterparts. Here, we study mechanisms controlling the electrochemical synthesis of CNTs from the capture and conversion of ambient CO 2 in molten salts and leverage this understanding to achieve the smallest-diameter CNTs ever reported in the literature from sustainable electrochemical synthesis routes, including some few-walled CNTs. Here, Fe catalyst layers are deposited at different thicknesses onto stainless steel to produce cathodes, and atomic layer deposition of Al 2 O 3 is performed on Ni to produce a corrosion-resistant anode. Our findings indicate a correlation between the CNT diameter and Fe metal layer thickness following electrochemical catalyst reduction at the cathode-molten salt interface. Further, catalyst coarsening during long duration synthesis experiments leads to a 2× increase in average diameters from 3 to 60 min durations, with CNTs produced after 3 min exhibiting a tight diameter distribution centered near ∼10 nm. Energy consumption analysis for the conversion of CO 2 into CNTs demonstrates energy input costs much lower than the value of CNTs-a concept that strictly requires and motivates small-diameter CNTs-and is more favorable compared to other costly CO 2 conversion techniques that produce lower-value materials and products.

  6. Formic Acid Oxidation over Hierarchical Porous Carbon Containing PtPd Catalysts

    Directory of Open Access Journals (Sweden)

    Elena Pastor

    2013-10-01

    Full Text Available The use of high surface monolithic carbon as support for catalysts offers important advantage, such as elimination of the ohmic drop originated in the interparticle contact and improved mass transport by ad-hoc pore design. Moreover, the approach discussed here has the advantage that it allows the synthesis of materials having a multimodal porous size distribution, with each pore size contributing to the desired properties. On the other hand, the monolithic nature of the porous support also imposes new challenges for metal loading. In this work, the use of Hierarchical Porous Carbon (HPC as support for PtPd nanoparticles was explored. Three hierarchical porous carbon samples (denoted as HPC-300, HPC-400 and HPC-500 with main pore size around 300, 400 and 500 nm respectively, are used as porous support. PtPd nanoparticles were loaded by impregnation and subsequent chemical reduction with NaBH4. The resulting material was characterized by EDX, XRD and conventional electrochemical techniques. The catalytic activity toward formic acid and methanol electrooxidation was evaluated by electrochemical methods, and the results compared with commercial carbon supported PtPd. The Hierarchical Porous Carbon support discussed here seems to be promising for use in DFAFC anodes.

  7. A Nitrogen-Doped Carbon Catalyst for Electrochemical CO2 Conversion to CO with High Selectivity and Current Density.

    Science.gov (United States)

    Jhong, Huei-Ru Molly; Tornow, Claire E; Smid, Bretislav; Gewirth, Andrew A; Lyth, Stephen M; Kenis, Paul J A

    2017-03-22

    We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO 2 to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H 2 (approximately 98 % CO and 2 % H 2 ), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=-1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm -2 . The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO 2 reduction as an approach to reduce atmospheric CO 2 emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  8. Supported zirconium sulfate on carbon nanotubes as water-tolerant solid acid catalyst

    International Nuclear Information System (INIS)

    Juan, Joon Ching; Jiang Yajie; Meng Xiujuan; Cao Weiliang; Yarmo, Mohd Ambar; Zhang Jingchang

    2007-01-01

    A new solid acid of zirconium sulfate (CZ) was successfully supported on carbon nanotube (CNT) for esterification reaction. Preparation conditions of the supported CZ have been investigated, to obtain highest catalytic activity for esterification reaction. XRD, TEM, BET, X-ray photoelectron spectra (XPS) and in situ FTIR analysis has also been carried out to understand the characteristics of the catalyst. In the esterification of acrylic acid with n-octanol, the supported CZ exhibited high catalytic activity and stability. The catalytic activity was nearly unchanged during four times of reuse. XRD and TEM analysis indicated that CZ was finely dispersed on CNT. XPS analysis shows that the CZ species was preserved and the chemical environment of the CZ has changed after loaded on CNT. This finding show that CNT as CZ support is an efficient water-tolerant solid acid

  9. Graphitized Carbon: A Promising Stable Cathode Catalyst Support Material for Long Term PEMFC Applications.

    Science.gov (United States)

    Mohanta, Paritosh Kumar; Regnet, Fabian; Jörissen, Ludwig

    2018-05-28

    Stability of cathode catalyst support material is one of the big challenges of polymer electrolyte membrane fuel cells (PEMFC) for long term applications. Traditional carbon black (CB) supports are not stable enough to prevent oxidation to CO₂ under fuel cell operating conditions. The feasibility of a graphitized carbon (GC) as a cathode catalyst support for low temperature PEMFC is investigated herein. GC and CB supported Pt electrocatalysts were prepared via an already developed polyol process. The physical characterization of the prepared catalysts was performed using transmission electron microscope (TEM), X-ray Powder Diffraction (XRD) and inductively coupled plasma optical emission spectrometry (ICP-OES) analysis, and their electrochemical characterizations were conducted via cyclic voltammetry(CV), rotating disk electrode (RDE) and potential cycling, and eventually, the catalysts were processed using membrane electrode assemblies (MEA) for single cell performance tests. Electrochemical impedance spectroscopy (EIS) and scanning electrochemical microscopy (SEM) have been used as MEA diagonostic tools. GC showed superior stability over CB in acid electrolyte under potential conditions. Single cell MEA performance of the GC-supported catalyst is comparable with the CB-supported catalyst. A correlation of MEA performance of the supported catalysts of different Brunauer⁻Emmett⁻Teller (BET) surface areas with the ionomer content was also established. GC was identified as a promising candidate for catalyst support in terms of both of the stability and the performance of fuel cell.

  10. Activation of peroxymonosulfate by graphitic carbon nitride loaded on activated carbon for organic pollutants degradation

    International Nuclear Information System (INIS)

    Wei, Mingyu; Gao, Long; Li, Jun; Fang, Jia; Cai, Wenxuan; Li, Xiaoxia; Xu, Aihua

    2016-01-01

    Highlights: • Supported g-C_3N_4 on AC catalysts with different loadings were prepared. • The metal free catalysts exhibited high efficiency for dyes degradation with PMS. • The catalyst presented a long-term stability for multiple runs. • The C=O groups played a key role in the oxidation process. - Abstract: Graphitic carbon nitride supported on activated carbon (g-C_3N_4/AC) was prepared through an in situ thermal approach and used as a metal free catalyst for pollutants degradation in the presence of peroxymonosulfate (PMS) without light irradiation. It was found that g-C_3N_4 was highly dispersed on the surface of AC with the increase of surface area and the exposition of more edges and defects. The much easier oxidation of C species in g-C_3N_4 to C=O was also observed from XPS spectra. Acid Orange 7 (AO7) and other organic pollutants could be completely degraded by the g-C_3N_4/AC catalyst within 20 min with PMS, while g-C_3N_4+PMS and AC+PMS showed no significant activity for the reaction. The performance of the catalyst was significantly influenced by the amount of g-C_3N_4 loaded on AC; but was nearly not affected by the initial solution pH and reaction temperature. In addition, the catalysts presented good stability. A nonradical mechanism accompanied by radical generation (HO· and SO_4·"−) in AO7 oxidation was proposed in the system. The C=O groups play a key role in the process; while the exposure of more N-(C)_3 group can further increase its electron density and basicity. This study can contribute to the development of green materials for sustainable remediation of aqueous organic pollutants.

  11. 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

    ). The supported Pt catalysts show significant improvement in catalytic activity towards the direct oxidation of methanol and DME, attributable to the enhanced adsorption and dehydrogenation of methanol and DME, as well as the presence of activated OH species in the catalysts. The latter is demonstrated......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...... to facilitate the removal of CO intermediates formed during the oxidation reactions....

  12. 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)

  13. Thermally oxidized aluminum as catalyst-support layer for vertically aligned single-walled carbon nanotube growth using ethanol

    Energy Technology Data Exchange (ETDEWEB)

    Azam, Mohd Asyadi, E-mail: asyadi@jaist.ac.jp [School of Materials Science, Japan Advanced Institute of Science and Technology (JAIST), 1-1 Asahidai, Nomi, Ishikawa 923-1292 (Japan); Fujiwara, Akihiko [Research and Utilization Division, Japan Synchrotron Radiation Research Institute (JASRI), 1-1-1, Kouto, Sayo-cho, Sayo, Hyogo 679-5198 (Japan); Shimoda, Tatsuya [School of Materials Science, Japan Advanced Institute of Science and Technology (JAIST), 1-1 Asahidai, Nomi, Ishikawa 923-1292 (Japan)

    2011-11-01

    Characteristics and role of Al oxide (Al-O) films used as catalyst-support layer for vertical growth of single-walled carbon nanotubes (SWCNTs) were studied. EB-deposited Al films (20 nm) were thermally oxidized at 400 deg. C (10 min, static air) to produce the most appropriate surface structure of Al-O. Al-O catalyst-support layers were characterized using various analytical measurements, i.e., atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), and spectroscopy ellipsometry (SE). The thermally oxidized Al-O has a highly roughened surface, and also has the most suitable surface chemical states compared to other type of Al-O support layers. We suggest that the surface of thermally oxidized Al-O characterized in this work enhanced Co catalyst activity to promote the vertically aligned SWCNT growth.

  14. Integrative CO2 Capture and Hydrogenation to Methanol with Reusable Catalyst and Amine: Toward a Carbon Neutral Methanol Economy.

    Science.gov (United States)

    Kar, Sayan; Sen, Raktim; Goeppert, Alain; Prakash, G K Surya

    2018-02-07

    Herein we report an efficient and recyclable system for tandem CO 2 capture and hydrogenation to methanol. After capture in an aqueous amine solution, CO 2 is hydrogenated in high yield to CH 3 OH (>90%) in a biphasic 2-MTHF/water system, which also allows for easy separation and recycling of the amine and catalyst for multiple reaction cycles. Between cycles, the produced methanol can be conveniently removed in vacuo. Employing this strategy, catalyst Ru-MACHO-BH and polyamine PEHA were recycled three times with 87% of the methanol producibility of the first cycle retained, along with 95% of catalyst activity after four cycles. CO 2 from dilute sources such as air can also be converted to CH 3 OH using this route. We postulate that the CO 2 capture and hydrogenation to methanol system presented here could be an important step toward the implementation of the carbon neutral methanol economy concept.

  15. Hydroprocessing catalyst development

    Energy Technology Data Exchange (ETDEWEB)

    Boorman, P.M.; Kydd, R.A.; Sorensen, T.S.; Chong, K.; Lewis, J.

    1992-08-01

    Co-Mo and Ni-Mo hydroprocessing catalysts were examined for their activity in removal of sulfur from thiophene in model compounds, and in the cracking and hydrocracking of cumene. Three types of support materials were examined: carbon, modified carbon, and carbon covered alumina. The objective of the study was to examine the correlation between catalyst activity in the hydrodenitrogenation of model compounds, and the resistance of the catalyst to nitrogen poisoning during use in the hydroprocessing of gas oils. The use of model compound testing provided information on the individual catalytic reactions promoted by those materials. Infrared spectroscopy was used to study surface species on the catalysts and to explain many of the trends in activity observed, revealing the role of fluoride and phosphorus as a secondary promoter. Testing of the catalysts in hydrotreating of gas oils allowed comparison of model compound results with those from a real feedstock. The gas oil was also spiked with a model nitrogen compound and the results from catalytic hydrotreating of this material were compared with those from unspiked material. A key finding was that the carbon supported catalysts were the most effective in treating high-nitrogen feeds. The very favorable deactivation properties of carbon and carbon-covered alumina supported catalysts make these promising from an industrial point of view where catalyst deactivation is a limiting factor. 171 refs., 25 figs., 43 tabs.

  16. ZIF-67 incorporated with carbon derived from pomelo peels: A highly efficient bifunctional catalyst for oxygen reduction/evolution reactions

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Hao; Yin, Feng-Xiang; Chen, Biao-Hua; He, Xiao-Bo; Lv, Peng-Liang; Ye, Cai-Yun; Liu, Di-Jia

    2017-05-01

    Developing carbon catalyst materials using natural, abundant and renewable resources as precursors plays an increasingly important role in clean energy generation and environmental protection. In this work, N-doped pomelo-peel-derived carbon (NPC) materials were prepared using a widely available food waste-pomelo peels and melamine. The synthetic NPC exhibits well-defined porosities and a highly doped-N content (e.g. 6.38 at% for NPC-2), therefore affords excellent oxygen reduction reaction (ORR) catalytic activities in alkaline electrolytes. NPC was further integrated with ZIF-67 to form ZIF-67@NPC hybrids through solvothermal reactions. The hybrid catalysts show substantially enhanced ORR catalytic activities comparable to that of commercial 20 wa Pt/C. Furthermore, the catalysts also exhibit excellent oxygen evolution reaction (OER) catalytic activities. Among all prepared ZIF-67@NPC hybrids, the optimal composition with ZIF-67 to NPC ratio of 2:1 exhibits the best ORR and OER bifunctional catalytic performance and the smallest Delta E (E-OER@10 mA cm(-2)-E-ORR@-1 mA cm(-2)) value of 0.79 V. The catalyst also demonstrated desirable 4-electron transfer pathways and superior catalytic stabilities. The Co-N-4 in ZIF-67, electrochemical active surface area, and the strong interactions between ZIF-67 and NPC are attributed as the main contributors to the bifunctional catalytic activities. These factors act synergistically, resulting in substantially enhanced bifunctional catalytic activities and stabilities; consequently, this hybrid catalyst is among the best of the reported bifunctional electrocatalysts and is promising for use in metal-air batteries and fuel cells. (C) 2016 Elsevier B.V. All rights reserved.

  17. Preparation of Carbon-Platinum-Ceria and Carbon-Platinum-Cerium catalysts and its application in Polymer Electrolyte Fuel Cell: Hydrogen, Methanol, and Ethanol

    Science.gov (United States)

    Guzman Blas, Rolando Pedro

    This thesis is focused on fuel cells using hydrogen, methanol and ethanol as fuel. Also, in the method of preparation of catalytic material for the anode: Supercritical Fluid Deposition (SFD) and impregnation method using ethylenediaminetetraacetic acid (EDTA) as a chelating agent. The first part of the thesis describes the general knowledge about Hydrogen Polymer Exchange Membrane Fuel Cell (HPEMFC),Direct Methanol Fuel Cell (DMFC) and Direct Ethanol Fuel Cell (DEFC), as well as the properties of Cerium and CeO2 (Ceria). The second part of the thesis describes the preparation of catalytic material by Supercritical Fluid Deposition (SFD). SFD was utilized to deposit Pt and ceria simultaneously onto gas diffusion layers. The Pt-ceria catalyst deposited by SFD exhibited higher methanol oxidation activity compared to the platinum catalyst alone. The linear sweep traces of the cathode made for the methanol cross over study indicate that Pt-Ceria/C as the anode catalyst, due to its better activity for methanol, improves the fuel utilization, minimizing the methanol permeation from anode to cathode compartment. The third and fourth parts of the thesis describe the preparation of material catalytic material Carbon-Platinum-Cerium by a simple and cheap impregnation method using EDTA as a chelating agent to form a complex with cerium (III). This preparation method allows the mass production of the material catalysts without additional significant cost. Fuel cell polarization and power curves experiments showed that the Carbon-Platinum-Cerium anode materials exhibited better catalytic activity than the only Vulcan-Pt catalysts for DMFC, DEFC and HPEMFC. In the case of Vulcan-20%Pt-5%w Cerium, this material exhibits better catalytic activity than the Vulcan-20%Pt in DMFC. In the case of Vulcan-40% Pt-doped Cerium, this material exhibits better catalytic activity than the Vulcan-40% Pt in DMFC, DEFC and HPEMFC. Finally, I propose a theory that explains the reason why the

  18. Activity of ruthenium, rhodium, iridium-ruthenium and iridium-rhodium adsorbed catalysts in dehydrogenation of formic acid

    Energy Technology Data Exchange (ETDEWEB)

    Mikhailov, V A; Zubovich, I A [Yaroslavskij Politekhnicheskij Inst. (USSR)

    1977-04-01

    The activity of Ru-, Rh- (Ir+nRu)- and (Ir+nRn) catalysts on sugar carbon and silicon dioxide in decomposition of HCOOH was studied. The catalyst activity increases in the series Iractivity is displayed by (Ir+nRh) catalysts on silicon dioxide. The results obtained point to activity of single centres (Ru)/sub 1/ and (Rh)/sub 1/ in the reaction of dehydration of HCOOH. It is shown that in the course of preparation of (Ir+nRh)- and (Ir+nRu)-catalysts the Ir atoms interact with Ru(Rh), and variable-composition structures are formed.

  19. Electrocatalytic properties of carbon-supported Pt-Ru catalysts with the high alloying degree for formic acid electrooxidation

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Yu.; Zhou, Yiming; Tang, Yawen; Lu, Tianhong [College of Chemistry and Environmental Science, Nanjing Normal University, Nanjing 210097 (China)

    2010-07-01

    A series of carbon-supported bimetallic Pt-Ru catalysts with high alloying degree and different Pt/Ru atomic ratio have been prepared by a chemical reduction method in the H{sub 2}O/ethanol/tetrahydrofuran (THF) mixture solvent. The structural and electronic properties of catalysts are characterized using X-ray reflection (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM). The electrooxidation of formic acid on these Pt-Ru nanoparticles are investigated by using cyclic voltammetry, chronoamperometry and CO-stripping measurements. The results of electrochemical measurements illustrate that the alloying degree and Pt/Ru atomic ratio of Pt-Ru catalyst play an important role in the electrocatalytic activity of the Pt-Ru/C catalyst for formic acid electrooxidation due to the bifunctional mechanism and the electronic effect. Since formic acid is an intermediate in the methanol electrooxidation on Pt electrode in acidic electrolyte, the observation provides an additional fundamental understanding of the structure-activity relationship of Pt-Ru catalyst for methanol electrooxidation. (author)

  20. Optimization of fuel cell membrane electrode assemblies for transition metal ion-chelating ordered mesoporous carbon cathode catalysts

    Directory of Open Access Journals (Sweden)

    Johanna K. Dombrovskis

    2014-12-01

    Full Text Available Transition metal ion-chelating ordered mesoporous carbon (TM-OMC materials were recently shown to be efficient polymer electrolyte membrane fuel cell (PEMFC catalysts. The structure and properties of these catalysts are largely different from conventional catalyst materials, thus rendering membrane electrode assembly (MEA preparation parameters developed for conventional catalysts not useful for applications of TM-OMC catalysts. This necessitates development of a methodology to incorporate TM-OMC catalysts in the MEA. Here, an efficient method for MEA preparation using TM-OMC catalyst materials for PEMFC is developed including effects of catalyst/ionomer loading and catalyst/ionomer-mixing and application procedures. An optimized protocol for MEA preparation using TM-OMC catalysts is described.

  1. Tungsten carbide/porous carbon composite as superior support for platinum catalyst toward methanol electro-oxidation

    International Nuclear Information System (INIS)

    Jiang, Liming; Fu, Honggang; Wang, Lei; Mu, Guang; Jiang, Baojiang; Zhou, Wei; Wang, Ruihong

    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 −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 BET ) of 457.92 m 2 g −1 . After loading Pt nanoparticles (NPs), the obtained Pt/WC/PC-35-1000 catalyst exhibits the highest unit mass electroactivity (595.93 A g −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

  2. 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.

  3. Microstructure, elastic, and inelastic properties of biomorphic carbons carbonized using a Fe-containing catalyst

    Science.gov (United States)

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

    2016-12-01

    The microstructure and amplitude dependences of the Young's modulus E and internal friction (logarithmic decrement δ), and microplastic properties of biocarbon matrices BE-C(Fe) obtained by beech tree carbonization at temperatures T carb = 850-1600°C in the presence of an iron-containing catalyst are studied. By X-ray diffraction analysis and transmission electron microscopy, it is shown that the use of Fe-catalyst during carbonization with T carb ≥ 1000°C leads to the appearance of a bulk graphite phase in the form of nanoscale bulk graphite inclusions in a quasi-amorphous matrix, whose volume fraction and size increase with T carb. The correlation of the obtained dependences E( T carb) and δ( T carb) with microstructure evolution with increasing T carb is revealed. It is found that E is mainly defined by a crystalline phase fraction in the amorphous matrix, i.e., a nanocrystalline phase at T carb 1300°C. Maximum values E = 10-12 GPa are achieved for samples with T carb ≈ 1150 and 1600°C. It is shown that the microplasticity manifest itself only in biocarbons with T carb ≥ 1300°C (upon reaching a significant volume of the graphite phase); in this case, the conditional microyield stress decreases with increasing total volume of introduced mesoporosity (free surface area).

  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. Patterned forests of vertically-aligned multiwalled carbon nanotubes using metal salt catalyst solutions.

    Science.gov (United States)

    Garrett, David J; Flavel, Benjamin S; Baronian, Keith H R; Downard, Alison J

    2013-01-01

    A simple method for producing patterned forests of multiwalled carbon nanotubes (MWCNTs) is described. An aqueous metal salt solution is spin-coated onto a substrate patterned with photoresist by standard methods. The photoresist is removed by acetone washing leaving the acetone-insoluble catalyst pattern on the substrate. Dense forests of vertically aligned (VA) MWCNTs are grown on the patterned catalyst layers by chemical vapour deposition. The procedures have been demonstrated by growing MWCNT forests on two substrates: silicon and conducting graphitic carbon films. The forests adhere strongly to the substrates and when grown directly on carbon film, offer a simple method of preparing MWCNT electrodes.

  6. 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

    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...

  7. Polymeric carbon nitride nanomesh as an efficient and durable metal-free catalyst for oxidative desulfurization.

    Science.gov (United States)

    Shen, Lijuan; Lei, Ganchang; Fang, Yuanxing; Cao, Yanning; Wang, Xinchen; Jiang, Lilong

    2018-03-06

    We report the first use of polymeric carbon nitride (CN) for the catalytic selective oxidation of H 2 S. The as-prepared CN with unique ultrathin "nanomeshes" structure exhibits excellent H 2 S conversion and high S selectivity. In particular, the CN nanomesh also displays better durability in the desulfurization reaction than traditional catalysts, such as carbon- and iron-based materials.

  8. Nitrogen–doped graphitized carbon shell encapsulated NiFe nanoparticles: A highly durable oxygen evolution catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Du, Lei; Luo, Langli; Feng, Zhenxing; Engelhard, Mark; Xie, Xiaohong; Han, Binghong; Sun, Junming; Zhang, Jianghao; Yin, Geping; Wang, Chongmin; Wang, Yong; Shao, Yuyan

    2017-09-01

    Oxygen evolution reaction (OER) plays a crucial role in various energy conversion devices such as water electrolyzers and metal–air batteries. Precious metal catalysts such as Ir, Ru and their oxides are usually used for enhancing reaction kinetics but are limited by their scarce resource. The challenges associated with alternative non–precious metal catalysts such as transition metal oxides and (oxy)hydroxides etc. are their low electronic conductivity and durability. Herein, we report a highly active (360 mV overpotential at 10 mA cm–2GEO) and durable (no degradation after 20000 cycles) OER catalyst derived from bimetallic metal–organic frameworks (MOFs) precursors. This catalyst consists of NiFe nanoparticles encapsulated by nitrogen–doped graphitized carbon shells. The electron-donation/deviation from Fe and tuned electronic structure of metal cores by Ni are revealed to be primary contributors to the enhanced OER activity, whereas N concentration contributes negligibly. We further demonstrated that the structure and morphology of encapsulating carbon shells, which are the key factors influencing the durability, are facilely controlled by the chemical state of precursors.

  9. A Comparative Study of Carbon Nanotubes Synthesized from Co/Zn/Al and Fe/Ni/Al Catalyst

    Directory of Open Access Journals (Sweden)

    Ezekiel Dixon Dikio

    2011-01-01

    Full Text Available The catalyst systems Fe/Ni/Al and Co/Zn/Al were synthesized and used in the synthesis of carbon nanotubes. The carbon nanotubes produced were characterized by Field Emission Scanning Electron Microscope (FE-SEM, Energy Dispersive x-ray Spectroscopy (EDS, Raman spectroscopy, Thermogravimetric Analysis (TGA and Transmission Electron Microscope (TEM. A comparison of the morphological profile of the carbon nanotubes produced from these catalysts indicates the catalyst system Fe/Ni/Al to have produced higher quality carbon nanotubes than the catalyst system Co/Zn/Al.

  10. High-surface-area active carbon

    International Nuclear Information System (INIS)

    O'Grady, T.M.; Wennerberg, A.N.

    1986-01-01

    This paper describes the preparation and properties of a unique active carbon having exceptionally high surface areas, over 2500 m 2 /gm, and extraordinary adsorptive capacities. The carbon is made by a direct chemical activation route in which petroleum coke or other carbonaceous sources are reacted with excess potassium hydroxide at 400 0 to 500 0 C to an intermediate product that is subsequently pyrolyzed at 800 0 to 900 0 C to active carbon containing potassium salts. These are removed by water washing and the carbon is dried to produce a powdered product. A granular carbon can also be made by further processing the powdered carbon by using specialized granulation techniques. Typical properties of the carbon include Iodine Numbers of 3000 to 3600, methylene blue adsorption of 650 to 750 mg/gm, pore volumes of 2.0 to 2.6 cc/gm and less than 3.0% ash. This carbon's high adsorption capacities make it uniquely suited for numerous demanding applications in the medical area, purifications, removal of toxic substances, as catalyst carriers, etc

  11. Metal-Carbon-CNF Composites Obtained by Catalytic Pyrolysis of Urban Plastic Residues as Electro-Catalysts for the Reduction of CO2

    Directory of Open Access Journals (Sweden)

    Jesica Castelo-Quibén

    2018-05-01

    Full Text Available Metal–carbon–carbon nanofibers composites obtained by catalytic pyrolysis of urban plastic residues have been prepared using Fe, Co or Ni as pyrolitic catalysts. The composite materials have been fully characterized from a textural and chemical point of view. The proportion of carbon nanofibers and the final content of carbon phases depend on the used pyrolitic metal with Ni being the most active pyrolitic catalysts. The composites show the electro-catalyst activity in the CO2 reduction to hydrocarbons, favoring all the formation of C1 to C4 hydrocarbons. The tendency of this activity is in accordance with the apparent faradaic efficiencies and the linear sweep voltammetries. The cobalt-based composite shows high selectivity to C3 hydrocarbons within this group of compounds.

  12. Activity and Stability of Dispersed Multi Metallic Pt-based Catalysts for CO Tolerance in Proton Exchange Membrane Fuel Cell Anodes.

    Science.gov (United States)

    Hassan, Ayaz; Ticianelli, Edson A

    2018-01-01

    Studies aiming at improving the activity and stability of dispersed W and Mo containing Pt catalysts for the CO tolerance in proton exchange membrane fuel cell (PEMFC) anodes are revised for the following catalyst systems: (1) a carbon supported PtMo electrocatalyst submitted to heat treatments; (2) Pt and PtMo nanoparticles deposited on carbon-supported molybdenum carbides (Mo2C/C); (3) ternary and quaternary materials formed by PtMoFe/C, PtMoRu/C and PtMoRuFe/C and; (4) Pt nanoparticles supported on tungsten carbide/carbon catalysts and its parallel evaluation with carbon supported PtW catalyst. The heat-treated (600 oC) Pt-Mo/C catalyst showed higher hydrogen oxidation activity in the absence and in the presence of CO and better stability, compared to all other Mo-containing catalysts. PtMoRuFe, PtMoFe, PtMoRu supported on carbon and Pt supported on Mo2C/C exhibited similar CO tolerances but better stability, as compared to as-prepared PtMo supported on carbon. Among the tungsten-based catalysts, tungsten carbide supported Pt catalyst showed reasonable performance and reliable stability in comparison to simple carbon supported PtW catalyst, though an uneven level of catalytic activity towards H2 oxidation in presence of CO is observed for the former as compared to Mo containing catalyst. However, a small dissolution of Mo, Ru, Fe and W from the anodes and their migration toward cathodes during the cell operation is observed. These results indicate that the fuel cell performance and stability has been improved but not yet totally resolved.

  13. Activity and Stability of Dispersed Multi Metallic Pt-based Catalysts for CO Tolerance in Proton Exchange Membrane Fuel Cell Anodes

    Directory of Open Access Journals (Sweden)

    AYAZ HASSAN

    2018-04-01

    Full Text Available ABSTRACT Studies aiming at improving the activity and stability of dispersed W and Mo containing Pt catalysts for the CO tolerance in proton exchange membrane fuel cell (PEMFC anodes are revised for the following catalyst systems: (1 a carbon supported PtMo electrocatalyst submitted to heat treatments; (2 Pt and PtMo nanoparticles deposited on carbon-supported molybdenum carbides (Mo2C/C; (3 ternary and quaternary materials formed by PtMoFe/C, PtMoRu/C and PtMoRuFe/C and; (4 Pt nanoparticles supported on tungsten carbide/carbon catalysts and its parallel evaluation with carbon supported PtW catalyst. The heat-treated (600 oC Pt-Mo/C catalyst showed higher hydrogen oxidation activity in the absence and in the presence of CO and better stability, compared to all other Mo-containing catalysts. PtMoRuFe, PtMoFe, PtMoRu supported on carbon and Pt supported on Mo2C/C exhibited similar CO tolerances but better stability, as compared to as-prepared PtMo supported on carbon. Among the tungsten-based catalysts, tungsten carbide supported Pt catalyst showed reasonable performance and reliable stability in comparison to simple carbon supported PtW catalyst, though an uneven level of catalytic activity towards H2 oxidation in presence of CO is observed for the former as compared to Mo containing catalyst. However, a small dissolution of Mo, Ru, Fe and W from the anodes and their migration toward cathodes during the cell operation is observed. These results indicate that the fuel cell performance and stability has been improved but not yet totally resolved.

  14. 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 (Gold nanoparticles (Au NP) possess unique reactive properties not present in the bulk state and have served in the past decade as a 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

  15. Production of 4He in D2-Loaded Palladium-Carbon Catalyst I

    International Nuclear Information System (INIS)

    Clarke, W. Brian

    2003-01-01

    A series of lead vials of internal volume 1.0 cm 3 were charged with ∼200 mg of carbon catalyst containing 0.5% Pd and 0.4% Pd. The vials were clamped to stainless steel manifolds on a vacuum line, then pumped out and filled with high-purity H 2 or D 2 at a pressure of 152 cm Hg and a temperature of 23 deg. C. Several vials contained ordinary activated carbon instead of palladium-carbon, and some vials contained only H 2 or D 2 . All the vials were stored in a sandbox heated to ∼ 200 deg. C for times up to 45 days before mass spectrometer measurements of 3 He and 4 He were made. No evidence was found for the high concentrations of 4 He claimed in similar experiments by several other researchers. The upper limit for the concentration excess of 4 He in D 2 in vials containing palladium-carbon is 11 ppt (parts per trillion) at the 95% confidence level. This limit for 4 He may be compared with previous claims in similar experiments of 100 ppm (parts per million) by Case and 11 ppm by George and McKubre et al

  16. Novel Catalyst for the Chirality Selective Synthesis of Single Walled Carbon Nanotubes

    Science.gov (United States)

    2015-05-12

    Final 3. DATES COVERED (From - To) 03-April-2013 to 02-April-2015 4. TITLE AND SUBTITLE Novel Catalyst for the Chirality Selective...Distribution is unlimited. 13. SUPPLEMENTARY NOTES 14. ABSTRACT Chiral single walled carbon nanotubes (SWCNTs) are known to possess unique... chirality control in SWCNT synthesis. A model catalyst based on CoSO4/SiO2 was developed that showed good selectivity to (9,8) nanotubes. Remote plasma

  17. Two Iron Complexes as Homogeneous and Heterogeneous Catalysts for the Chemical Fixation of Carbon Dioxide.

    Science.gov (United States)

    Karan, Chandan Kumar; Bhattacharjee, Manish

    2018-04-16

    Two new bimetallic iron-alkali metal complexes of amino acid (serine)-based reduced Schiff base ligand were synthesized and structurally characterized. Their efficacy as catalysts for the chemical fixation of carbon dioxide was explored. The heterogeneous version of the catalytic reaction was developed by the immobilization of these homogeneous bimetallic iron-alkali metal complexes in an anion-exchange resin. The resin-bound complexes can be used as recyclable catalysts up to six cycles.

  18. Effect of reverse Boudouard reaction catalyst on the performance of solid oxide carbon fuel cells integrated with a dry gasifier

    International Nuclear Information System (INIS)

    Kim, Sun-Kyung; Mehran, Muhammad Taqi; Mushtaq, Usman; Lim, Tak-Hyoung; Lee, Jong-Won; Lee, Seung-Bok; Park, Seok-Joo; Song, Rak-Hyun

    2016-01-01

    Highlights: • The addition of K_2CO_3 catalyst in carbon fuel improves the performance of SO-CFC. • Thermal and electrochemical analyses done to elucidate the catalytic enhancement. • Material characterization of SO-CFC performed after long-term degradation test. - Abstract: A solid oxide carbon fuel cell (SO-CFC) integrated with a dry gasifier was operated on activated carbon fuel and the effect of adding a reverse Boudouard gasification catalyst on the performance and long-term operation characteristics of the SO-CFC was investigated. The reactivity of the carbon fuels for the Boudouard gasification reaction was analyzed by a thermal analysis at various operating conditions. The SO-CFC was then operated on gasified fuel gas consisting of CO_2 and CO obtained from the integrated dry gasifier. The SO-CFC operated on activated carbon fuel with 5 wt.% K_2CO_3 achieved a maximum power density of 202, 262, and 271 mW/cm"2 at 750, 800, and 850 °C, respectively; the SO-CFC fueled with activated carbon fuel without a catalyst meanwhile yielded maximum power density of 168 mW/cm"2 at 850 °C. By using electrochemical impedance spectroscopy, the effect of adding the catalyst on the gasification products and subsequently on the performance of the SO-CFC was studied. A long-term degradation test was conducted by continuously operating the SO-CFC at 50 mA/cm"2 for 518 h at 750 °C. During the long-term degradation test, the average degradation rate of the SO-CFC was found to be 183 mV/kh. The post-mortem SEM and XRD analyses of the SO-CFC after the long-term test revealed the presence of carbon deposits and oxidation of Ni at the anode, causing a relatively higher degree of degradation in the SO-CFC integrated with the dry gasifier during the long-term operation. The addition of the K_2CO_3 based dry gasification catalyst significantly enhances the performance of the SO-CFC integrated with dry gasification, but during long-term operation, the degradation rate is found

  19. 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.

  20. Mass-produced multi-walled carbon nanotubes as catalyst supports for direct methanol fuel cells.

    Science.gov (United States)

    Jang, In Young; Park, Ki Chul; Jung, Yong Chae; Lee, Sun Hyung; Song, Sung Moo; Muramatsu, Hiroyuki; Kim, Yong Jung; Endo, Morinobu

    2011-01-01

    Commercially mass-produced multi-walled carbon nanotubes, i.e., VGNF (Showa Denko Co.), were applied to support materials for platinum-ruthenium (PtRu) nanoparticles as anode catalysts for direct methanol fuel cells. The original VGNFs are composed of high-crystalline graphitic shells, which hinder the favorable surface deposition of the PtRu nanoparticles that are formed via borohydride reduction. The chemical treatment of VGNFs with potassium hydroxide (KOH), however, enables highly dispersed and dense deposition of PtRu nanoparticles on the VGNF surface. This capability becomes more remarkable depending on the KOH amount. The electrochemical evaluation of the PtRu-deposited VGNF catalysts showed enhanced active surface areas and methanol oxidation, due to the high dispersion and dense deposition of the PtRu nanoparticles. The improvement of the surface deposition states of the PtRu nanoparticles was significantly due to the high surface area and mesorporous surface structure of the KOH-activated VGNFs.

  1. Soot oxidation over NOx storage catalysts. Activity and deactivation

    International Nuclear Information System (INIS)

    Krishna, K.; Makkee, M.

    2006-01-01

    Soot oxidation activity and deactivation of NO x storage and reduction (NSR) catalysts containing Pt, K, and Ba supported on Al 2 O 3 , are studied under a variety of reaction conditions. K-containing catalysts decrease soot oxidation temperature with O 2 alone and the presence of Pt further enhance the activity due to synergetic effect. The active species responsible for synergism on Pt/K-Al 2 O 3 are unstable and cannot be regenerated. Soot oxidation temperature decreases by about 150 o C with NO+O 2 exhaust feed gas and under lean conditions NSR system acts as catalysed soot filter (CSF). The reactions that are mainly responsible for decreasing soot oxidation temperature are: (1) soot oxidation with NO 2 followed by NO recycles to NO 2 , and (2) soot oxidation with O 2 assisted by NO 2 . Only a part of the stored NO x that is decomposed at high temperatures under lean conditions is found to be useful for soot oxidation. NO x storage capacity of NSR catalysts decreases upon ageing under soot oxidising conditions. This will lead to a decreased soot oxidation activity on stored nitrate decomposition. Pt/K-Al 2 O 3 catalyst is more active, but least stable compared with Pt/Ba-Al 2 O 3 . (author)

  2. Carbon-supported co-pyridine as non-platinum cathode catalyst for alkaline membrane fuel cells

    International Nuclear Information System (INIS)

    Qiao, Jinli; Xu, Li; Liu, Yuyu; Xu, Pan; Shi, Jingjing; Liu, Shiyao; Tian, Binglun

    2013-01-01

    Development of high-performance cost-effective electrocatalyts that can replace Pt catalyst have been a central theme in polymer electrolyte membrane fuel cells (PEMFCs) including direct methanol fuel cells (DMFCs). Here we show that carbon-supported pyridine–cobalt nanoparticles (CoPy/C) can generate a high catalytic activity toward the oxygen reduction reaction (ORR). The catalysts are synthesized using cobalt sulfate heptahydrate (CoSO 4 ·7H 2 O) and pyridine (Py) as the Co and N precursors via a solid state reaction by heat-treatment in an inert atmosphere at 800 °C. In particular, the ORR kinetics on these catalyst materials are evaluated using rotating disk electrode (RDE) technique in electrolytes of various KOH concentrations, ranging from 0.05 to 12 M. The Koutecky–Levich equation analyses indicate that the transferred electron number, n, per oxygen molecule on CoPy/C electrode depend on the low negative ovevrpotentials in low KOH concentrations, whereas in high KOH concentrations the values of n for oxygen reduction depend on the high negative overpotentials, and varies between 3.5 and 4.0. These catalysts exhibit the superior methanol tolerance to commercial 40%Pt/C catalyst, and the negative effect of high KOH concentration is much less for CoPy/C than for Pt/C, suggesting the promising utilization of CoPy/C as electrocatalysts for alkaline polymer electrolyte membrane fuel cells

  3. Coupling of Carbon Dioxide with Epoxides Efficiently Catalyzed by Thioether-Triphenolate Bimetallic Iron(III) Complexes: Catalyst Structure-Reactivity Relationship and Mechanistic DFT Study

    KAUST Repository

    Della Monica, Francesco; Vummaleti, Sai V. C.; Buonerba, Antonio; Nisi, Assunta De; Monari, Magda; Milione, Stefano; Grassi, Alfonso; Cavallo, Luigi; Capacchione, Carmine

    2016-01-01

    A series of dinuclear iron(III)I complexes supported by thioether-triphenolate ligands have been prepared to attain highly Lewis acidic catalysts. In combination with tetrabutylammonium bromide (TBAB) they are highly active catalysts in the synthesis of cyclic organic carbonates through the coupling of carbon dioxide to epoxides with the highest initial turnover frequencies reported to date for the conversion of propylene oxide to propylene carbonate for iron-based catalysts (5200h-1; 120°C, 2MPa, 1h). In particular, these complexes are shown to be highly selective catalysts for the coupling of carbon dioxide to internal oxiranes affording the corresponding cyclic carbonates in good yield and with retention of the initial stereochemical configuration. A density functional theory (DFT) investigation provides a rational for the relative high activity found for these Fe(III) complexes, showing the fundamental role of the hemilabile sulfur atom in the ligand skeleton to promote reactivity. Notably, in spite of the dinuclear nature of the catalyst precursor only one metal center is involved in the catalytic cycle. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  4. Coupling of Carbon Dioxide with Epoxides Efficiently Catalyzed by Thioether-Triphenolate Bimetallic Iron(III) Complexes: Catalyst Structure-Reactivity Relationship and Mechanistic DFT Study

    KAUST Repository

    Della Monica, Francesco

    2016-08-25

    A series of dinuclear iron(III)I complexes supported by thioether-triphenolate ligands have been prepared to attain highly Lewis acidic catalysts. In combination with tetrabutylammonium bromide (TBAB) they are highly active catalysts in the synthesis of cyclic organic carbonates through the coupling of carbon dioxide to epoxides with the highest initial turnover frequencies reported to date for the conversion of propylene oxide to propylene carbonate for iron-based catalysts (5200h-1; 120°C, 2MPa, 1h). In particular, these complexes are shown to be highly selective catalysts for the coupling of carbon dioxide to internal oxiranes affording the corresponding cyclic carbonates in good yield and with retention of the initial stereochemical configuration. A density functional theory (DFT) investigation provides a rational for the relative high activity found for these Fe(III) complexes, showing the fundamental role of the hemilabile sulfur atom in the ligand skeleton to promote reactivity. Notably, in spite of the dinuclear nature of the catalyst precursor only one metal center is involved in the catalytic cycle. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  5. Polymer-modified copper catalysts on carbon-containing support for reactions of H2O2 decomposition and cyclohexane oxidation

    Directory of Open Access Journals (Sweden)

    S. Auezkhanova

    2012-12-01

    Full Text Available Polymer-copper catalysts supported on a carbon-containing sorbent(CS, obtained by rice husk pyrolysis have been studied in the reactions of hydrogen peroxide decomposition and cyclohexane oxidation by hydrogen peroxide at 40°C and atmospheric pressure. The effect of the polymer nature on the activity of the developed catalysts have been shown. Polyhexamethyleneguanidine (PHMG was an optimal modifier for the developed catalysts. The calculated number of catalytic cycles (TON for 7% Cu-PGMG/CS was 450.

  6. Co-deposition of Pt and ceria anode catalyst in supercritical carbon dioxide for direct methanol fuel cell applications

    International Nuclear Information System (INIS)

    You, Eunyoung; Guzmán-Blas, Rolando; Nicolau, Eduardo; Aulice Scibioh, M.; Karanikas, Christos F.; Watkins, James J.; Cabrera, Carlos R.

    2012-01-01

    Pt and mixed Pt-ceria catalysts were deposited onto gas diffusion layers using supercritical fluid deposition (SFD) to fabricate thin layer electrodes for direct methanol fuel cells. Dimethyl (1,5-cyclooctadiene) platinum (II) (CODPtMe 2 ) and tetrakis (2,2,6,6-tetramethyl 3,5-heptanedionato) cerium (IV) (Ce(tmhd) 4 ) were used as precursors. Hydrogen-assisted Pt deposition was performed in compressed carbon dioxide at 60 °C and 17.2 MPa to yield high purity Pt on carbon-black based gas diffusion layers. During the preparation of the mixed Pt-ceria catalyst, hydrogen reduction of CODPtMe 2 to yield Pt catalyzed the deposition of ceria from Ce(tmhd) 4 enabling co-deposition at 150 °C. The catalyst layers were characterized using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electron microscope-energy dispersive spectral (SEM-EDS) analyses. Their electrochemical performance toward methanol oxidation was examined in half cell mode using a three electrode assembly as well as in fuel cell mode. The thin layer electrodes formed via SFD exhibited higher performance in fuel cell operations compared to those prepared by the conventional brush-paint method. Furthermore, the Pt-ceria catalyst with an optimized composition exhibited greater methanol oxidation activity than pure platinum.

  7. 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%.

  8. Fabrication of magnetic carbon composites from peanut shells and its application as a heterogeneous Fenton catalyst in removal of methylene blue

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Lincheng, E-mail: zhoulc@lzu.edu.cn; Ma, Junjun; Zhang, He; Shao, Yanming; Li, Yanfeng

    2015-01-01

    Graphical abstract: Peanut shell magnetic carbon (PMC) were fabricated by carbonized the mixture of peanut shells and (NH{sub 4}){sub 3}Fe(C{sub 2}O{sub 4}){sub 3}. The obtained PMC exhibit high efficiency in catalysis oxidation methylene blue with the help of K{sub 2}S{sub 2}O{sub 8} and it can be easily separated from aqueous by external magnetic field. Meanwhile, the catalyst can be reused for seven times almost without decreased of activity. - Highlights: • Novel peanut shell magnetic carbon (PMC) catalysts were successfully synthesized. • PMC exhibited superior activity as a heterogeneous Fenton-like catalyst. • A high efficient Fenton-like system was set up for removal MB. • PMC posed excellent catalysis oxidation quality, stability and good reusability. - Abstract: Magnetic carbons were prepared from agricultural waste peanut shells and Ferric ammonium oxalate via a simple impregnation and carbonization process. The obtained composites were characterized by element analysis, MÖssbauer spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, X-ray diffraction, vibrating sample magnetometry and the Brunauer-Emmett-Teller surface area method, respectively. The magnetic carbon material was used as catalyst of heterogeneous Fenton reaction to remove methylene blue with the help of persulfate in waste water. The results indicated that both the removal rate and removal efficiency of this catalytic system are very excellent. The degradation efficiency was best (90% within 30 min) using initial concentrations of 0.5 g L{sup −1} persulfate and 40 mg L{sup −1} methylene blue. The removal mechanism was investigated by LC-MS. The catalyst retained its activity after seven reuses, indicating its good stability and reusability. It is inexpensive because it consists mainly of agricultural waste. Its porosity contributed to its high activity, which was achieved without any additional activation process. These indicating that the catalyst is

  9. The activation mechanism of Fe-based olefin metathesis catalysts

    KAUST Repository

    Poater, Albert

    2014-08-01

    Density functional theory calculations have been used to describe the first turnover for olefin metathesis reaction of a homogenous Fe-based catalyst bearing a N-heterocyclic carbene ligand with methoxyethene as a substrate. Equal to conventional Ru-based catalysts, the activation of its Fe congener occurs through a dissociative mechanism, however with a more exothermic reaction energy profile. Predicted upper energy barriers were calculated to be on average ∼2 kcal/mol more beneficial for Fe catalyzed metathesis. Overall, this present computational study emphasises on advantages of Fe-based metathesis and gives a potential recipe for the design of an efficient Fe-based olefin metathesis catalysts. © 2014 Elsevier B.V.

  10. The activation mechanism of Fe-based olefin metathesis catalysts

    KAUST Repository

    Poater, Albert; Pump, Eva; Vummaleti, Sai V. C.; Cavallo, Luigi

    2014-01-01

    Density functional theory calculations have been used to describe the first turnover for olefin metathesis reaction of a homogenous Fe-based catalyst bearing a N-heterocyclic carbene ligand with methoxyethene as a substrate. Equal to conventional Ru-based catalysts, the activation of its Fe congener occurs through a dissociative mechanism, however with a more exothermic reaction energy profile. Predicted upper energy barriers were calculated to be on average ∼2 kcal/mol more beneficial for Fe catalyzed metathesis. Overall, this present computational study emphasises on advantages of Fe-based metathesis and gives a potential recipe for the design of an efficient Fe-based olefin metathesis catalysts. © 2014 Elsevier B.V.

  11. Ethanol electrooxidation on novel carbon supported Pt/SnOx/C catalysts with varied Pt:Sn ratio

    International Nuclear Information System (INIS)

    Jiang, L.; Colmenares, L.; Jusys, Z.; Sun, G.Q.; Behm, R.J.

    2007-01-01

    Novel carbon supported Pt/SnO x /C catalysts with Pt:Sn atomic ratios of 5:5, 6:4, 7:3 and 8:2 were prepared by a modified polyol method and characterized with respect to their structural properties (X-ray diffraction (XRD) and transmission electron microscopy (TEM)), chemical composition (XPS), their electrochemical properties (base voltammetry, CO ad stripping) and their electrocatalytic activity and selectivity for ethanol oxidation (ethanol oxidation reaction (EOR)). The data show that the Pt/SnO x /C catalysts are composed of Pt and tin oxide nanoparticles with an average Pt particle diameter of about 2 nm. The steady-state activity of the Pt/SnO x /C catalysts towards the EOR decreases with tin content at room temperature, but increases at 80 deg. C. On all Pt/SnO x /C catalysts, acetic acid and acetaldehyde represent dominant products, CO 2 formation contributes 1-3% for both potentiostatic and potentiodynamic reaction conditions. With increasing potential, the acetaldehyde yield decreases and the acetic acid yield increases. The apparent activation energies of the EOR increase with tin content (19-29 kJ mol -1 ), but are lower than on Pt/C (32 kJ mol -1 ). The somewhat better performance of the Pt/SnO x /C catalysts compared to alloyed PtSn x /C catalysts is attributed to the presence of both sufficiently large Pt ensembles for ethanol dehydrogenation and C-C bond splitting and of tin oxide for OH generation. Fuel cell measurements performed for comparison largely confirm the results obtained in model studies

  12. Recent progress in solution plasma-synthesized-carbon-supported catalysts for energy conversion systems

    Science.gov (United States)

    Lun Li, Oi; Lee, Hoonseung; Ishizaki, Takahiro

    2018-01-01

    Carbon-based materials have been widely utilized as the electrode materials in energy conversion and storage technologies, such as fuel cells and metal-air batteries. In these systems, the oxygen reduction reaction is an important step that determines the overall performance. A novel synthesis route, named the solution plasma process, has been recently utilized to synthesize various types of metal-based and heteroatom-doped carbon catalysts. In this review, we summarize cutting-edge technologies involving the synthesis and modeling of carbon-supported catalysts synthesized via solution plasma process, followed by current progress on the electrocatalytic performance of these catalysts. This review provides the fundamental and state-of-the-art performance of solution-plasma-synthesized electrode materials, as well as the remaining scientific and technological challenges for this process.

  13. 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

    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...

  14. Modeling of carbon monoxide oxidation kinetics over NASA carbon dioxide laser catalysts

    Science.gov (United States)

    Herz, Richard K.

    1989-01-01

    The recombination of CO and O2 formed by the dissociation of CO2 in a sealed CO2 laser discharge zone is examined. Conventional base-metal-oxide catalysts and conventional noble-metal catalysts are not effective in recombining the low O2/CO ratio at the low temperatures used by the lasers. The use of Pt/SnO2 as the noble-metal reducible-oxide (NMRO), or other related materials from Group VIIIA and IB and SnO2 interact synergistically to produce a catalytic activity that is substantially higher than either componet separately. The Pt/SnO2 and Pd/SnO2 were reported to have significant reaction rates at temperatures as low as -27 C, conditions under which conventional catalysts are inactive. The gas temperature range of lasers is 0 + or - 40 C. There are three general ways in which the NMRO composite materials can interact synergistically: one component altering the properties of another component; the two components each providing independent catalytic functions in a complex reaction mechanism; and the formation of catalytic sites through the combination of two components at the atomic level. All three of these interactions may be important in low temperature CO oxidation over NMRO catalysts. The effect of the noble metal on the oxide is discussed first, followed by the effect of the oxide on the noble metal, the interaction of the noble metal and oxide to form catalytic sites, and the possible ways in which the CO oxidation reaction is catalyzed by the NMRO materials.

  15. Transesterification of Jatropha oil with dimethyl carbonate to produce fatty acid methyl ester over reusable Ca–La–Al mixed-oxide catalyst

    International Nuclear Information System (INIS)

    Syamsuddin, Y.; Murat, M.N.; Hameed, B.H.

    2015-01-01

    Highlights: • Transesterification of Jatropha oil over CaO-based catalyst. • Physicochemical properties of the synthesized catalyst. • Best reaction condition for FAME synthesis. • The catalyst showed high activity and stability for transesterification with Jatropha oil. - Abstract: Jatropha oil (JO) was transesterified with dimethyl carbonate (DMC) to produce fatty acid methyl ester (FAME) over synthesized Ca–La–Al mixed-oxide catalyst. The influence of different parameters on transesterification of Jatropha oil was investigated in a batch reactor. These parameters included reaction temperature (110–160 °C), reaction time (30–240 min), DMC-to-oil molar ratio (4:1–18:1) and catalyst loading amount (1–10 wt.%, based on the oil weight). The mixed-oxide catalyst with a molar ratio of 6:2:1 (Ca–La–Al) showed high catalytic activity for FAME synthesis. More than 90% of FAME was obtained under the following reaction conditions: 150 °C, reaction temperature; 180 min, reaction time; 15:1, DMC-to-oil molar ratio; and 7 wt.% amount of catalyst loading. The catalyst also exhibited high stability and could be reused for up to five cycles with less than 5% yield reduction per cycle.

  16. Confined-interface-directed synthesis of Palladium single-atom catalysts on graphene/amorphous carbon

    DEFF Research Database (Denmark)

    Xi, Jiangbo; Sun, Hongyu; Zhang, Zheye

    2018-01-01

    The maximized atomic efficiency of supported catalysts is highly desired in heterogeneous catalysis. Therefore, the design and development of active, stable, and atomic metal-based catalysts remains a formidable challenge. To tackle these problems, it is necessary to investigate the interaction b...

  17. Effects of composition on structure and activity of PtRu/C catalysts.

    Science.gov (United States)

    Wiltshire, Richard J K; King, Colin R; Rose, Abigail; Wells, Peter P; Davies, Hazel; Hogarth, Martin P; Thompsett, David; Theobald, Brian; Mosselmans, Fredrick W; Roberts, Mark; Russell, Andrea E

    2009-04-07

    A series of carbon supported PtRu bimetallic catalysts with varying Pt:Ru ratio were prepared and characterised using ex situ and in situ XRD, in situ EXAFS at 0 V vs. RHE, ex situ XPS and monolayer CO stripping voltammetry. Although the catalysts were found to be well mixed/alloyed, with no evidence of unalloyed Ru (oxides) present, the surfaces of the electrocatalyst nanoparticles were found to be enriched with Pt compared to the nominal bulk composition. The methanol oxidation activities of the catalysts were determined in 1.0 mol dm(-3) H2SO4. In agreement with published studies of polycrystalline bulk PtRu alloys the catalyst with a 0.6 surface fraction of Pt was found to give the best methanol oxidation activity at 30 degrees C. However, at 80 degrees C a greater surface fraction of Ru could be tolerated, with some activity at low current densities found for a Pt surface fraction as low as 0.2. The results support the conclusion that a limited amount of methanol dehydrogenation occurs at Ru sites or Ru dominated surface ensembles at 80 degrees C.

  18. Pyrolysis-catalysis of waste plastic using a nickel-stainless-steel mesh catalyst for high-value carbon products.

    Science.gov (United States)

    Zhang, Yeshui; Nahil, Mohamad A; Wu, Chunfei; Williams, Paul T

    2017-11-01

    A stainless-steel mesh loaded with nickel catalyst was produced and used for the pyrolysis-catalysis of waste high-density polyethylene with the aim of producing high-value carbon products, including carbon nanotubes (CNTs). The catalysis temperature and plastic-to-catalyst ratio were investigated to determine the influence on the formation of different types of carbon deposited on the nickel-stainless-steel mesh catalyst. Increasing temperature from 700 to 900°C resulted in an increase in the carbon deposited on the nickel-loaded stainless-steel mesh catalyst from 32.5 to 38.0 wt%. The increase in sample-to-catalyst ratio reduced the amount of carbon deposited on the mesh catalyst in terms of g carbon g -1 plastic. The carbons were found to be largely composed of filamentous carbons, with negligible disordered (amorphous) carbons. Transmission electron microscopy analysis of the filamentous carbons revealed them to be composed of a large proportion (estimated at ∼40%) multi-walled carbon nanotubes (MWCNTs). The optimum process conditions for CNT production, in terms of yield and graphitic nature, determined by Raman spectroscopy, was catalysis temperature of 800°C and plastic-to-catalyst ratio of 1:2, where a mass of 334 mg of filamentous/MWCNTs g -1 plastic was produced.

  19. Detection of airborne carbon nanotubes based on the reactivity of the embedded catalyst.

    Science.gov (United States)

    Neubauer, N; Kasper, G

    2015-01-01

    A previously described method for detecting catalyst particles in workplace air((1,2)) was applied to airborne carbon nanotubes (CNT). It infers the CNT concentration indirectly from the catalytic activity of metallic nanoparticles embedded as part of the CNT production process. Essentially, one samples airborne CNT onto a filter enclosed in a tiny chemical reactor and then initiates a gas-phase catalytic reaction on the sample. The change in concentration of one of the reactants is then determined by an IR sensor as measure of activity. The method requires a one-point calibration with a CNT sample of known mass. The suitability of the method was tested with nickel containing (25 or 38% by weight), well-characterized multi-walled CNT aerosols generated freshly in the lab for each experiment. Two chemical reactions were investigated, of which the oxidation of CO to CO2 at 470°C was found to be more effective, because nearly 100% of the nickel was exposed at that temperature by burning off the carbon, giving a linear relationship between CO conversion and nickel mass. Based on the investigated aerosols, a lower detection limit of 1 μg of sampled nickel was estimated. This translates into sampling times ranging from minutes to about one working day, depending on airborne CNT concentration and catalyst content, as well as sampling flow rate. The time for the subsequent chemical analysis is on the order of minutes, regardless of the time required to accumulate the sample and can be done on site.

  20. Synthesis of Carbon Nano tubes Using Anadara Granosa Shells as Catalyst Support

    International Nuclear Information System (INIS)

    Mohd Zobir Hussein; Mohd Zobir Hussein; Salwani Asyikin Zakarya; Siti Halimah Sarijo

    2011-01-01

    The synthesis of carbon nano tubes (CNTs) by chemical vapor deposition (CVD) method using natural calcite prepared from Anadara granosa shells (CS), as metal catalyst support was studied. Hexane and iron were used as carbon precursor and catalyst, respectively. The as synthesised CNTs was characterized using XRD, TEM and FESEM. From the XRD patterns the CNTs peak can be seen more incisive after purification process and from the FESEM micrographs the CNTs can be seen as a bunch of rope-like structures. (author)

  1. Graphitised Carbon Nanofibres as Catalyst Support for PEMFC

    DEFF Research Database (Denmark)

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

    2011-01-01

    (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...

  2. Synthesis of dimethyl carbonate (DMC) by oxidative carbonylation of methanol using polymer-supported CuCl{sub 2} catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Sato, Y. [Daicel Chemical Industries, Ltd., Hyogo (Japan). Research Center; Kobe University, Kobe (Japan); Kagotani, M. [Daicel Chemical Industries, Ltd., Hyogo (Japan). Research Center; Soma, Y. [Osaka National Research Institute, Osaka (Japan)

    2000-01-01

    Polymer, including 2,2'-bipyridine, poly(4-methyl-4'-vinyl-2,2'-bipyridine)(Pvbpy), was investigated for the synthesis of dimethyl carbonate (DMC) as a support for CuCl{sub 2}, by oxidative carbonylation of methanol in the liquid-phase. The CuCl{sub 2} complex (Pvbpy-CuCl{sub 2}) was insoluble in methanol, and the reaction system was heterogeneous. The Pvbpy-CuCl{sub 2} catalyst showed considerable catalytic activity (DMC yield: 44.4 % and DMC selectivity: 9206 %, at methanol conversion: 1.79 %), which is comparable to the previously reported data of poly (vinylpyridine) (PVP)-CuCl{sub 2} catalyst; the Pvbpy-CuCl{sub 2} catalyst could be recycled after filtration and washing thrice, provided, not having lost activity. The corrosion originating from Cl{sup -} was greatly improved by immobilizing the CuCl{sub 2} by Pvbpy. Elimination of CuCl{sub 2} from the Pvbpy support was observed during the reaction. In the first reaction, about 38 % of the initially supported Cl was released, and in the second and the third reactions, most of the Cl was retained. The rate of corrosion of stainless steels in the first use of the catalyst (0.6 mg h{sup -1} for HC276) was greater than that in the rate of the second and the third uses (<0.1 mg h{sup -1}). These results are closely related to the amount of Cl{sup -} released from the Pvbpy support, which demonstrates that the main cause of corrosion in the catalytic system is Cl{sup -} released from the Pvbpy-CuCl{sub 2} catalyst. From XPS study of the catalyst, it became obvious that Cu(2) was gradually reduced to Cu(1) during the reaction. (author)

  3. 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

  4. Controlling thin film structure for the dewetting of catalyst nanoparticle arrays for subsequent carbon nanofiber growth

    International Nuclear Information System (INIS)

    Randolph, S J; Fowlkes, J D; Melechko, A V; Klein, K L; III, H M Meyer; Simpson, M L; Rack, P D

    2007-01-01

    Vertically aligned carbon nanofiber (CNF) growth is a catalytic chemical vapor deposition process in which structure and functionality is controlled by the plasma conditions and the properties of the catalyst nanoparticles that template the fiber growth. We have found that the resultant catalyst nanoparticle network that forms by the dewetting of a continuous catalyst thin film is dependent on the initial properties of the thin film. Here we report the ability to tailor the crystallographic texture and composition of the nickel catalyst film and subsequently the nanoparticle template by varying the rf magnetron sputter deposition conditions. After sputtering the Ni catalyst thin films, the films are heated and exposed to an ammonia dc plasma, to chemically reduce the native oxide on the films and induce dewetting of the film to form nanoparticles. Subsequent nanoparticle treatment in an acetylene plasma at high substrate temperature results in CNF growth. Evidence is presented that the texture and composition of the nickel thin film has a significant impact on the structure and composition of the formed nanoparticle, as well as the resultant CNF morphology. Nickel films with a preferred (111) or (100) texture were produced and conditions favoring interfacial silicidation reactions were identified and investigated. Both compositional and structural analysis of the films and nanoparticles indicate that the properties of the as-deposited Ni catalyst film influences the subsequent nanoparticle formation and ultimately the catalytic growth of the carbon nanofibers

  5. High Performance Fe- and N- Doped Carbon Catalyst with Graphene Structure for Oxygen Reduction

    Science.gov (United States)

    Peng, Hongliang; Mo, Zaiyong; Liao, Shijun; Liang, Huagen; Yang, Lijun; Luo, Fan; Song, Huiyu; Zhong, Yiliang; Zhang, Bingqing

    2013-05-01

    Proton exchange membrane fuel cells are promising candidates for a clean and efficient energy conversion in the future, the development of carbon based inexpensive non-precious metal ORR catalyst has becoming one of the most attractive topics in fuel cell field. Herein we report a Fe- and N- doped carbon catalyst Fe-PANI/C-Mela with graphene structure and the surface area up to 702 m2 g-1. In 0.1 M HClO4 electrolyte, the ORR onset potential for the catalyst is high up to 0.98 V, and the half-wave potential is only 60 mV less than that of the Pt/C catalyst (Loadings: 51 μg Pt cm-2). The catalyst shows high stability after 10,000 cyclic voltammetry cycles. A membrane electrode assembly made with the catalyst as a cathode is tested in a H2-air single cell, the maximum power density reached ~0.33 W cm2 at 0.47 V.

  6. Magnetic porous Fe3O4/carbon octahedra derived from iron-based metal-organic framework as heterogeneous Fenton-like catalyst

    Science.gov (United States)

    Li, Wenhui; Wu, Xiaofeng; Li, Shuangde; Tang, Wenxiang; Chen, Yunfa

    2018-04-01

    The synthesis of effective and recyclable Fenton-like catalyst is still a key factor for advanced oxidation processes. Herein, magnetic porous Fe3O4/carbon octahedra were constructed by a two-step controlled calcination of iron-based metal organic framework. The porous octahedra were assembled by interpenetrated Fe3O4 nanoparticles coated with graphitic carbon layer, offering abundant mesoporous channels for the solid-liquid contact. Moreover, the oxygen-containing functional groups on the surface of graphitic carbon endow the catalysts with hydrophilic nature and well-dispersion into water. The porous Fe3O4/carbon octahedra show efficiently heterogeneous Fenton-like reactions for decomposing the organic dye methylene blue (MB) with the help of H2O2, and nearly 100% removal efficiency within 60 min. Furthermore, the magnetic catalyst retains the activity after ten cycles and can be easily separated by external magnetic field, indicating the long-term catalytic durability and recyclability. The good Fenton-like catalytic performance of the as-synthesized Fe3O4/carbon octahedra is ascribed to the unique mesoporous structure derived from MOF-framework, as well as the sacrificial role and stabilizing effect of graphitic carbon layer. This work provides a facile strategy for the controllable synthesis of integrated porous octahedral structure with graphitic carbon layer, and thereby the catalyst holds significant potential for wastewater treatment.

  7. 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.

  8. Effect of iron catalyst thickness on vertically aligned carbon nanotube forest straightness for CNT-MEMS

    International Nuclear Information System (INIS)

    Moulton, Kellen; Jensen, Brian D; Morrill, Nicholas B; Konneker, Adam M; Vanfleet, Richard R; Allred, David D; Davis, Robert C

    2012-01-01

    This paper examines the effect of iron catalyst thickness on the straightness of growth of carbon nanotubes (CNTs) for microelectromechanical systems fabricated using the CNT-templated-microfabrication (CNT-M) process. SEM images of samples grown using various iron catalyst thicknesses show that both straight sidewalls and good edge definition are achieved using an iron thickness between 7 and 8 nm. Below this thickness, individual CNTs are well aligned, but the sidewalls of CNT forests formed into posts and long walls are not always straight. Above this thickness, the CNT forest sidewalls are relatively straight, but edge definition is poor, with significantly increased sidewall roughness. The proximity of a device or feature to other regions of iron catalyst also affects CNT growth. By using an iron catalyst thickness appropriate for straight growth, and by adding borders of iron around features or devices, a designer can greatly improve straightness of growth for CNT-MEMS. (paper)

  9. Platinum catalyst formed on carbon nanotube by the in-liquid plasma method for fuel cell

    Energy Technology Data Exchange (ETDEWEB)

    Show, Yoshiyuki; Hirai, Akira; Almowarai, Anas; Ueno, Yutaro

    2015-12-01

    In-liquid plasma was generated in the carbon nanotube (CNT) dispersion fluid using platinum electrodes. The generated plasma spattered the surface of the platinum electrodes and dispersed platinum particles into the CNT dispersion. Therefore, the platinum nanoparticles were successfully formed on the CNT surface in the dispersion. The platinum nanoparticles were applied to the proton exchange membrane fuel cell (PEMFC) as a catalyst. The electrical power of 108 mW/cm{sup 2} was observed from the fuel cell which was assembled with the platinum catalyst formed on the CNT by the in-liquid plasma method. - Highlights: • The platinum catalyst was successfully formed on the CNT surface in the dispersion by the in-liquid plasma method. • The electrical power of 108 mW/cm{sup 2} was observed from the fuel cell which was assembled with the platinum catalyst formed on the CNT by the in-liquid plasma method.

  10. Methanol-Tolerant Platinum-Palladium Catalyst Supported on Nitrogen-Doped Carbon Nanofiber for High Concentration Direct Methanol Fuel Cells.

    Science.gov (United States)

    Kim, Jiyoung; Jang, Jin-Sung; Peck, Dong-Hyun; Lee, Byungrok; Yoon, Seong-Ho; Jung, Doo-Hwan

    2016-08-15

    Pt-Pd catalyst supported on nitrogen-doped carbon nanofiber (N-CNF) was prepared and evaluated as a cathode electrode of the direct methanol fuel cell (DMFC). The N-CNF, which was directly synthesized by the catalytic chemical vapor deposition from acetonitrile at 640 °C, was verified as having a change of electrochemical surface properties such as oxygen reduction reaction (ORR) activities and the electrochemical double layer compared with common carbon black (CB). To attain the competitive oxygen reduction reaction activity with methanol tolerance, the Pt and Pd metals were supported on the CB or the N-CNF. The physical and electrochemical characteristics of the N-CNF-supported Pt-Pd catalyst were examined and compared with catalyst supported on the CB. In addition, DMFC single cells using these catalysts as the cathode electrode were applied to obtain I-V polarization curves and constant current operating performances with high-concentration methanol as the fuel. Pt-Pd catalysts had obvious ORR activity even in the presence of methanol. The higher power density was obtained at all the methanol concentrations when it applied to the membrane electrode assembly (MEA) of the DMFC. When the N-CNF is used as the catalyst support material, a better performance with high-concentration methanol is expected.

  11. Methanol-Tolerant Platinum-Palladium Catalyst Supported on Nitrogen-Doped Carbon Nanofiber for High Concentration Direct Methanol Fuel Cells

    Directory of Open Access Journals (Sweden)

    Jiyoung Kim

    2016-08-01

    Full Text Available Pt-Pd catalyst supported on nitrogen-doped carbon nanofiber (N-CNF was prepared and evaluated as a cathode electrode of the direct methanol fuel cell (DMFC. The N-CNF, which was directly synthesized by the catalytic chemical vapor deposition from acetonitrile at 640 °C, was verified as having a change of electrochemical surface properties such as oxygen reduction reaction (ORR activities and the electrochemical double layer compared with common carbon black (CB. To attain the competitive oxygen reduction reaction activity with methanol tolerance, the Pt and Pd metals were supported on the CB or the N-CNF. The physical and electrochemical characteristics of the N-CNF–supported Pt-Pd catalyst were examined and compared with catalyst supported on the CB. In addition, DMFC single cells using these catalysts as the cathode electrode were applied to obtain I-V polarization curves and constant current operating performances with high-concentration methanol as the fuel. Pt-Pd catalysts had obvious ORR activity even in the presence of methanol. The higher power density was obtained at all the methanol concentrations when it applied to the membrane electrode assembly (MEA of the DMFC. When the N-CNF is used as the catalyst support material, a better performance with high-concentration methanol is expected.

  12. Active sites of ligand-protected Au25 nanoparticle catalysts for CO2 electroreduction to CO

    Science.gov (United States)

    Alfonso, Dominic R.; Kauffman, Douglas; Matranga, Christopher

    2016-05-01

    Recent experimental studies have reported the electrochemical reduction of carbon dioxide (CO2) into CO at atomically precise negatively charged Au25- nanoclusters. The studies showed CO2 conversion at remarkably low overpotentials, but the exact mechanisms and nature of the active sites remain unclear. We used first-principles density functional theory and continuum solvation models to examine the role of the cluster during electrochemical CO2 reduction and analyze the free energies of proposed intermediate species. Contrary to previous assumptions, our results show that the fully ligand protected cluster is not an active CO2 reduction catalyst because formation of the crucial carboxyl intermediate required very high electrochemical potentials. Instead, our calculations suggest that the reduction process likely occurs on a dethiolated gold site, and adsorbed carboxyl intermediate formation was significantly stabilized at dethiolated gold sites. These findings point to the crucial role of exposed metal sites during electrochemical CO2 reduction at gold nanocluster catalysts.

  13. Microstructural study of Ni/γ-Al2O3 catalyst: addition effects of CeO2 on carbon dioxide reforming of methane

    International Nuclear Information System (INIS)

    Valentini, Antoninho; Probst, Luiz Fernando Dias; Carreno, Neftali L. V.; Leite, Edson R.; Pontes, Fenelon M.; Longo, Elson; Schreiner, Wido H.; Lisboa-Filho, Paulo N.

    2003-01-01

    The carbon dioxide reforming of methane was carried out over nickel catalysts supported on the γ-Al 2 O 3 /CeO 2 system prepared by wet impregnation. With the increase of the Co2 weight in the catalyst, a higher stability was observed in the catalytic activity, together with an excellent resistance to carbon deposition and a better Ni dispersion. The catalysts were characterized by means of surface area measurements, TPR, H 2 chemisorption, XRD, SEM, EDX, XPS and TEM. An interaction between Ni and CeO 2 was observed to the Ni/CeO 2 sample after activation in a H 2 atmosphere above 300 deg C. Such behavior has a significantly influence on the catalytic activity. (author)

  14. Preparation of Pt–Ru bimetallic catalyst supported on carbon ...

    Indian Academy of Sciences (India)

    Unknown

    of carbon nanotube (Iijima 1991) was first based on the carbon-arc method, though the carbon nanotube prepared by this method are more graphitic, the low yield and rela- tively small length (< 1 m) make the production cost very high. The template synthesis method (Martin 1994) and catalytic production methods (Jose et ...

  15. Synthesis and Electrochemical Evaluation of Carbon Supported Pt-Co Bimetallic Catalysts Prepared by Electroless Deposition and Modified Charge Enhanced Dry Impregnation

    Directory of Open Access Journals (Sweden)

    John Meynard M. Tengco

    2016-06-01

    Full Text Available Carbon-supported bimetallic Pt-Co cathode catalysts have been previously identified as higher activity alternatives to conventional Pt/C catalysts for fuel cells. In this work, a series of Pt-Co/C catalysts were synthesized using electroless deposition (ED of Pt on a Co/C catalyst prepared by modified charge enhanced dry impregnation. X-ray diffraction (XRD and scanning transmission electron microscopy (STEM characterization of the base catalyst showed highly dispersed particles. A basic ED bath containing PtCl62− as the Pt precursor, dimethylamine borane as reducing agent, and ethylenediamine as stabilizing agent successfully targeted deposition of Pt on Co particles. Simultaneous action of galvanic displacement and ED resulted in Pt-Co alloy formation observed in XRD and energy dispersive X-ray spectroscopy (XEDS mapping. In addition, fast deposition kinetics resulted in hollow shell Pt-Co alloy particles while particles with Pt-rich shell and Co-rich cores formed with controlled Pt deposition. Electrochemical evaluation of the Pt-Co/C catalysts showed lower active surface but much higher mass and surface activities for oxygen reduction reaction compared to a commercial Pt/C fuel cell catalyst.

  16. A surface science model for the Phillips ethylene polymerization catalyst : thermal activation and polymerization activity

    NARCIS (Netherlands)

    Kimmenade, van E.M.E.; Kuiper, A.E.T.; Tamminga, Y.; Thuene, P.C.; Niemantsverdriet, J.W.

    2004-01-01

    A series of CrOx/SiO2/Si(100) model catalysts were tested for ethylene polymerization activity, varying chromium loading, and calcination temperature. Chromium coverage of the model catalyst, quantified by Rutherford backscattering spectrometry, decreases with increasing calcination temperature as

  17. Highly Active Non-PGM Catalysts Prepared from Metal Organic Frameworks

    Directory of Open Access Journals (Sweden)

    Heather M. Barkholtz

    2015-06-01

    Full Text Available Finding inexpensive alternatives to platinum group metals (PGMs is essential for reducing the cost of proton exchange membrane fuel cells (PEMFCs. Numerous materials have been investigated as potential replacements of Pt, of which the transition metal and nitrogen-doped carbon composites (TM/Nx/C prepared from iron doped zeolitic imidazolate frameworks (ZIFs are among the most active ones in catalyzing the oxygen reduction reaction based on recent studies. In this report, we demonstrate that the catalytic activity of ZIF-based TM/Nx/C composites can be substantially improved through optimization of synthesis and post-treatment processing conditions. Ultimately, oxygen reduction reaction (ORR electrocatalytic activity must be demonstrated in membrane-electrode assemblies (MEAs of fuel cells. The process of preparing MEAs using ZIF-based non-PGM electrocatalysts involves many additional factors which may influence the overall catalytic activity at the fuel cell level. Evaluation of parameters such as catalyst loading and perfluorosulfonic acid ionomer to catalyst ratio were optimized. Our overall efforts to optimize both the catalyst and MEA construction process have yielded impressive ORR activity when tested in a fuel cell system.

  18. Efficient strategy to Cu/Si catalyst into vertically aligned carbon ...

    Indian Academy of Sciences (India)

    Abstract. Bamboo-shaped vertically aligned carbon nanotubes (bs-VACNTs) were fabricated on Cu/Si catalyst by ... on Si wafer material when compared to the other commer- ..... [3] Li H, Zhao N, He C, Shi C, Du X, Li J and Cui Q 2008 Mater.

  19. 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...

  20. Effect of catalyst preparation on the yield of carbon nanotube growth

    International Nuclear Information System (INIS)

    Escobar, Mariano; Rubiolo, Gerardo; Candal, Roberto; Goyanes, Silvia

    2009-01-01

    Multi-wall carbon nanotubes (MWCNTs) were synthesized by catalytic chemical vapor deposition (CVD) on catalytic iron nanoparticles dispersed in a silica matrix, prepared by sol gel method. In this contribution, variation of gelation condition on catalyst structure and its influence on the yield of carbon nanotubes growth was studied. The precursor utilized were tetraethyl-orthosilicate and iron nitrate. The sols were dried at two different temperatures in air (25 or 80 deg. C) and then treated at 450 deg. C for 10 h. The xerogels were introduced into the chamber and reduced in a hydrogen/nitrogen (10%v/v) atmosphere at 600 deg. C. MWCNTs were formed by deposition of carbon atoms from decomposition of acetylene at 700 deg. C. The system gelled at RT shows a yield of 100% respect to initial catalyst mass whereas the yield of that gelled at 80 deg. C was lower than 10%. Different crystalline phases are observed for both catalysts in each step of the process. Moreover, TPR analysis shows that iron oxide can be efficiently reduced to metallic iron only in the system gelled at room temperature. Carbon nanotubes display a diameter of about 25-40 nm and several micron lengths. The growth mechanism of MWCNTs is base growth mode for both catalysts.

  1. Effect of catalyst preparation on the yield of carbon nanotube growth

    Energy Technology Data Exchange (ETDEWEB)

    Escobar, Mariano, E-mail: mescobar@df.uba.a [Dep. Quimica Inorganica, Analitica y Quimica Fisica, FCEyN, UBA, Ciudad Universitaria (1428), Bs As (Argentina); LP and MC, Dep. Fisica, FCEyN, UBA (Argentina); Rubiolo, Gerardo [Unidad de Actividad Materiales, CNEA, Av Gral Paz 1499, San Martin (1650), Bs As (Argentina); Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) (Argentina); Candal, Roberto [Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) (Argentina); Instituto de Fisico-quimica de Materiales, Ambiente y Energia (INQUIMAE), CONICET - UBA (Argentina); Goyanes, Silvia [LP and MC, Dep. Fisica, FCEyN, UBA (Argentina); Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) (Argentina)

    2009-10-01

    Multi-wall carbon nanotubes (MWCNTs) were synthesized by catalytic chemical vapor deposition (CVD) on catalytic iron nanoparticles dispersed in a silica matrix, prepared by sol gel method. In this contribution, variation of gelation condition on catalyst structure and its influence on the yield of carbon nanotubes growth was studied. The precursor utilized were tetraethyl-orthosilicate and iron nitrate. The sols were dried at two different temperatures in air (25 or 80 deg. C) and then treated at 450 deg. C for 10 h. The xerogels were introduced into the chamber and reduced in a hydrogen/nitrogen (10%v/v) atmosphere at 600 deg. C. MWCNTs were formed by deposition of carbon atoms from decomposition of acetylene at 700 deg. C. The system gelled at RT shows a yield of 100% respect to initial catalyst mass whereas the yield of that gelled at 80 deg. C was lower than 10%. Different crystalline phases are observed for both catalysts in each step of the process. Moreover, TPR analysis shows that iron oxide can be efficiently reduced to metallic iron only in the system gelled at room temperature. Carbon nanotubes display a diameter of about 25-40 nm and several micron lengths. The growth mechanism of MWCNTs is base growth mode for both catalysts.

  2. 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...

  3. Highly active thermally stable nanoporous gold catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Biener, Juergen; Wittstock, Arne; Biener, Monika M.; Bagge-Hansen, Michael; Baeumer, Marcus; Wichmann, Andre; Neuman, Bjoern

    2016-12-20

    In one embodiment, a system includes a nanoporous gold structure and a plurality of oxide particles deposited on the nanoporous gold structure; the oxide particles are characterized by a crystalline phase. In another embodiment, a method includes depositing oxide nanoparticles on a nanoporous gold support to form an active structure and functionalizing the deposited oxide nanoparticles.

  4. Structure and Reactivity of Zeolite- and Carbon-Supported Catalysts for the Oxidative Carbonylation of Alcohols

    OpenAIRE

    Briggs, Daniel Neal

    2010-01-01

    AbstractStructure and Reactivity of Zeolite- and Carbon-Supported Catalysts for the Oxidative Carbonylation of AlcoholsbyDaniel Neal BriggsDoctor of Philosophy in Chemical EngineeringUniversity of California, BerkeleyProfessor Alexis T. Bell, Chair The oxidative carbonylation of alcohols to produce dialkyl carbonates is a process that takes place commercially in a slurry of cuprous chloride in the appropriate alcohol. While this process is chemically efficient, it incurs costs in terms of ene...

  5. High yield growth of patterned vertically aligned carbon nanotubes using inkjet-printed catalyst.

    Science.gov (United States)

    Beard, James D; Stringer, Jonathan; Ghita, Oana R; Smith, Patrick J

    2013-10-09

    This study reports on the fabrication of vertically aligned carbon nanotubes localized at specific sites on a growth substrate by deposition of a nanoparticle suspension using inkjet printing. Carbon nanotubes were grown with high yield as vertically aligned forests to a length of approximately 400 μm. The use of inkjet printing for catalyst fabrication considerably improves the production rate of vertically aligned patterned nanotube forests compared with conventional patterning techniques, for example, electron beam lithography or photolithography.

  6. Synthesis of gold nano-catalysts supported on carbon nanotubes by using electroless plating technique

    International Nuclear Information System (INIS)

    Ma Xicheng; Li Xia; Lun Ning; Wen Shulin

    2006-01-01

    Gold nanoparticles supported on carbon nanotubes were prepared by using electroless plating technique. High-resolution transmission electron microscopy (HRTEM) has shown that spherical gold nanoparticles were homogeneously dispersed on the surfaces of the carbon nanotubes with a distribution of particle sizes sharply at around 3-4 nm in diameter. The results presented in this work will probably provide new catalysts with better performances

  7. Carbon tetrachloride desorption from activated carbon

    International Nuclear Information System (INIS)

    Jonas, L.A.; Sansone, E.B.

    1981-01-01

    Carbon tetrachloride was desorbed from a granular activated carbon subsequent to its adsorption under various vapor exposure periods. The varied conditions of exposure resulted in a range of partially saturated carbon beds which, when followed by a constant flow rate for desorption, generated different forms of the desorbing concentration versus time curve. A method of analyzing the desorption curves is presented which permits extraction of the various desorbing rates from the different desorption and to relate this to the time required for such regeneration. The Wheeler desorption kinetic equation was used to calculate the pseudo first order desorption rate constant for the carbon. The desorption rate constant was found to increase monotonically with increasing saturation of the bed, permitting the calculation of the maximum desorption rate constant for the carbon at 100% saturation. The Retentivity Index of the carbon, defined as the dimensionless ratio of the adsorption to the desorption rate constant, was found to be 681

  8. Highly active Ni/Y-doped ZrO{sub 2} catalysts for CO{sub 2} methanation

    Energy Technology Data Exchange (ETDEWEB)

    Takano, H., E-mail: takano_hi@hitachizosen.co.jp [Hitachi Zosen Corporation, Kashiwa, 277-8515 (Japan); Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo, 060-8628 (Japan); Kirihata, Y.; Izumiya, K.; Kumagai, N. [Hitachi Zosen Corporation, Kashiwa, 277-8515 (Japan); Habazaki, H., E-mail: habazaki@eng.hokudai.ac.jp [Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo, 060-8628 (Japan); Division of Applied Chemistry & Frontier Chemistry Center, Faculty of Engineering, Hokkaido University, Sapporo, 060-8628 (Japan); Hashimoto, K. [Tohoku Institute of Technology, Sendai, 277-8515 (Japan)

    2016-12-01

    Highlights: • The Ni/Y-doped ZrO{sub 2} catalysts show highly catalytic activity for CO{sub 2} methanation. • Bidentate carbonate is a major adsorption spice on the Ni/Y-doped ZrO{sub 2} catalysts. • The oxide support of t-ZrO{sub 2} and/or c-ZrO{sub 2} with oxygen vacancies plays a key role. - Abstract: The catalytic methanation of CO{sub 2} was carried out on Ni catalysts supported on Y-doped ZrO{sub 2} with various Y{sup 3+} concentrations and Ni/(Zr + Y) molar ratio = 1. The catalysts were characterized by X-ray diffraction, scanning transmission electron microscopy, specific surface area, temperature-programmed desorption of CO{sub 2}, and temperature-programmed reaction. In addition, operando diffuse-reflectance infrared Fourier-transform spectroscopy (DRIFT) was used to identify the adsorbed reaction intermediate. Catalysts supported on Y-doped ZrO{sub 2} show higher catalytic activity than the catalyst on Y-free ZrO{sub 2} with a monoclinic ZrO{sub 2} phase. The catalytic activity is also dependent upon the Y{sup 3+} concentration, and the highest activity was obtained for the catalyst with a Y/(Zr + Y) molar ratio of 0.333, which consists mainly of fcc Ni and cubic ZrO{sub 2} phase. Y{sup 3+} doping into ZrO{sub 2} introduces oxygen vacancies, which play an important role in enhancing the catalytic activity. The operando DRIFT study reveals that a CO adsorption intermediate is absent, and bidentate carbonate is an important intermediate for CH{sub 4} formation.

  9. The role of the iron catalyst in the toxicity of multi-walled carbon nanotubes (MWCNTs).

    Science.gov (United States)

    Visalli, Giuseppa; Facciolà, Alessio; Iannazzo, Daniela; Piperno, Anna; Pistone, Alessandro; Di Pietro, Angela

    2017-09-01

    This study aimed to investigate the role of iron, used as a catalyst, in the biological response to pristine and functionalized multi-walled carbon nanotubes (p/fMWCNTs) with an iron content of 2.5-2.8%. Preliminarily, we assessed the pro-oxidant activity of MWCNTs-associated iron by an abiotic test. To evaluate iron bioavailability, we measured intracellular redox-active iron in A549 cells exposed to both MWCNT suspensions and to the cell medium preconditioned by MWCNTs, in order to assess the iron dissolution rate under physiological conditions. Moreover, in exposed cells, we detected ROS levels, 8-oxo-dG and mitochondrial function. The results clearly highlighted that MWCNTs- associated iron was not redox-active and that iron leakage did not occur under physiological conditions, including the oxidative burst of specialized cells. Despite this, in MWCNTs exposed cells, higher level of intracellular redox-active iron was measured in comparison to control and a significant time-dependent ROS increase was observed (P<0.01). Higher levels of 8-oxo-dG, a marker of oxidative DNA damage, and decreased mitochondrial function, confirmed the oxidative stress induced by MWCNTs. Based on the results we believe that oxidative damage could be attributable to the release of endogenous redox-active iron. This was due to the damage of acidic vacuolar compartment caused by endocytosis-mediated MWCNT internalization. Copyright © 2017 Elsevier GmbH. All rights reserved.

  10. MORE ACTIVE AND SULFUR RESISTANT BIMETALLIC Pd-Ni CATALYSTS

    OpenAIRE

    Betti, Carolina; Carrara, Nicolás; Badano, Juan; Lederhos, Cecilia; Vera, Carlos; Quiroga, Mónica

    2018-01-01

    The influence of the kind of metal precursor and the sequence of impregnation on the properties of Pd-Ni catalysts was evaluated during the test reaction of selective hydrogenation of styrene to ethylbenzene by means of physicochemical characterization. The focus was put on the final hydrogenating activity and the resistance to deactivation by sulfided compounds (thiophene). The used techniques of characterization were ICP, XPS, XDR, TPR, CO chemisorption and TEM. XPS results indicated the pr...

  11. Alkali resistant Ni-loaded yolk-shell catalysts for direct internal reforming in molten carbonate fuel cells

    Science.gov (United States)

    Jang, Won-Jun; Hong, Young Jun; Kim, Hak-Min; Shim, Jae-Oh; Roh, Hyun-Seog; Kang, Yun Chan

    2017-06-01

    A facile and scalable spray pyrolysis process is applied to synthesize multi-shelled Ni-loaded yolk-shell catalysts on various supports (Al2O3, CeO2, ZrO2, and La(OH)3). The prepared catalysts are applied to direct internal reforming (DIR) in a molten carbonate fuel cell (MCFC). Even on exposure to alkali hydroxide vapors, the Ni-loaded yolk-shell catalysts remain highly active for DIR-MCFCs. The Ni@Al2O3 microspheres show the highest conversion (92%) of CH4 and the best stability among the prepared Ni-loaded yolk-shell catalysts. Although the initial CH4 conversion of the Ni@ZrO2 microspheres is higher than that of the Ni@CeO2 microspheres, the Ni@CeO2 microspheres are more stable. The catalytic performance is strongly dependent on the surface area and acidity and also partly dependent on the reducibility. The acidic nature of Al2O3 combined with its high surface area and yolk-shell structure enhances the adsorption of CH4 and resistance against alkali poisoning, resulting in efficient DIR-MCFC reactions.

  12. A facile self-assembly approach to prepare palladium/carbon nanotubes catalyst for the electro-oxidation of ethanol

    Science.gov (United States)

    Wen, Cuilian; Zhang, Xinyuan; Wei, Ying; Zhang, Teng; Chen, Changxin

    2018-02-01

    A facile self-assembly approach is reported to prepare palladium/carbon nanotubes (Pd/CNTs) catalyst for the electro-oxidation of ethanol. In this method, the Pd-oleate/CNTs was decomposed into the Pd/CNTs at an optimal temperature of 195 °C in air, in which no inert gas is needed for the thermal decomposition process due to the low temperature used and the decomposed products are also environmental friendly. The prepared Pd/CNTs catalyst has a high metallic Pd0 content and the Pd particles in the catalyst are disperse, uniform-sized with an average size of ˜2.1 nm, and evenly distributed on the CNTs. By employing our strategy, the problems including the exfoliation of the metal particles from the CNTs and the aggregation of the metal particles can be solved. Comparing with the commercial Pd/C one, the prepared Pd/CNTs catalyst exhibits a much higher electrochemical activity and stability for the electro-oxidation of ethanol in the direct ethanol fuel cells.

  13. High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst

    KAUST Repository

    Zheng, Yao; Jiao, Yan; Zhu, Yihan; Li, Lu Hua; Han, Yu; Chen, Ying; Jaroniec, Mietek; Qiao, Shi Zhang

    2016-01-01

    Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.

  14. High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst.

    Science.gov (United States)

    Zheng, Yao; Jiao, Yan; Zhu, Yihan; Li, Lu Hua; Han, Yu; Chen, Ying; Jaroniec, Mietek; Qiao, Shi-Zhang

    2016-12-14

    Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.

  15. High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst

    KAUST Repository

    Zheng, Yao

    2016-11-28

    Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.

  16. Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol

    DEFF Research Database (Denmark)

    Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank

    2014-01-01

    The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO 2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO...... 2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO 2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni......-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni 5 Ga 3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al 2 O 3 catalysts revealed the same or better methanol synthesis activity, as well as considerably...

  17. 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.)

  18. Carbon monoxide tolerant anodes for proton exchange membrane (PEM) fuel cells. 1. Catalyst development approach

    Energy Technology Data Exchange (ETDEWEB)

    Holleck, G L; Pasquariello, D M; Clauson, S L

    1998-07-01

    PEM fuel cells are highly attractive for distributed power and cogeneration systems. They are efficient and function virtually without noise or pollution. To be competitive PEM fuel cells must operate on fuel mixtures obtained by reforming of widely available natural gas or liquid hydrocarbons. Reformed fuel gas mixtures invariably contain CO, a strong poison for Pt. Therefore CO tolerant anode catalysts are essential for wide spread PEMFC introduction. It is the objective to develop effective CO tolerant fuel cell catalysts based on multi-component platinum-transition metal alloys. Towards this goal the authors have developed a novel approach for the synthesis and performance evaluation of multifunctional ternary alloy fuel cell catalysts. The alloys are prepared as well-defined thin films on standard TFE-bonded carbon substrates via a dc magnetron sputtering technique. The anodes are laminated to Nafion membranes and the electrochemical performance is measured in a representative fuel cell configuration with H{sub 2} and H{sub 2}/CO gas mixtures. The multi-target sputtering technique permits one to reproducibly synthesize true alloy films of controlled composition. The deposit morphology and electrode structure are determined by the standardized TFE bonded carbon substrate. The thin catalyst layer is concentrated at the electrode ionomer interface where it can be fully utilized in a representative fuel cell configuration. Thus, a true comparative fuel cell catalyst evaluation is possible. The effectiveness of this approach will be demonstrated with Pt, Pt-Ru and Pt-Ru-X catalyzed anodes.

  19. Facile synthesis of porous graphene-like carbon nitride nanosheets with high surface area and enhanced photocatalytic activity via one-step catalyst-free solution self-polymerization

    Science.gov (United States)

    Wu, Shikai; Wen, Shengwu; Xu, Xinmei; Huang, Guozhi; Cui, Yifan; Li, Jinyu; Qu, Ailan

    2018-04-01

    Porous graphite carbon nitride nanosheets (g-C3N4) are achieved via one-step catalyst-free solution self-polymerization from a single melamine precursor. The resultant porous g-C3N4 nanosheets with the best photodegradation capacity provided the surface area of 669.15 m2/g, which is superior to the surface area of any other porous g-C3N4 reported. Results showed enhanced adsorption and degradation capacity of methyl orange (MO) under UV-visible light irradiation (λ > 350 nm) compared to bulk g-C3N4. The MO oxidation of the porous g-C3N4 nanosheets is driven mostly by the participation of holes, and secondly by rad O2- and rad OH radicals. This approach shed lights on porous g-C3N4 production simply by self-polycondensation of single functional monomer. It also provided a low-cost and eco-friendly method to facilely mass-produce g-C3N4 nanosheets with high surface area for many potential applications.

  20. Preparation and characterization of the perovskite catalysts : activity studies for diesel surrogate (dodecane) reforming

    Energy Technology Data Exchange (ETDEWEB)

    Kondakindi, R.; Kundu, A.; Karan, K.; Peppley, B. [Queen' s-RMC Fuel Cell Research Centre, Kingston, ON (Canada)

    2009-07-01

    Canada's northern communities rely on diesel fuel for generating electricity. The process of converting diesel to electricity in internal combustion engines is not efficient and generates significant amounts of unwanted products. This paper presented an alternative process whereby diesel is reformed into hydrogen-rich reformate which can then be fed to a solid oxide fuel cell. This alternative process converts energy more efficiently and eliminates the formation of nitrogen oxides (NOx) and soot. This study focused on the development of LaFeO{sub 3} based perovskite catalysts for diesel reforming. The activity of the perovskite catalysts was assessed for steam reforming of dodecane, a surrogate for diesel. In order to study the effect on catalytic activity, various perovskite materials were prepared by doping the perovskite at A-site to minimize the coke deposition and at B-site to improve the activity. Preliminary results for dodecane reforming for selected perovskites were promising. Additional testing is underway regarding catalyst activity and stability studies as well carbon and sulphur poisoning.

  1. Functionalized carbon nanofibers as solid acid catalysts for transesterification

    NARCIS (Netherlands)

    Stellwagen, D.R.; van der Klis, Frits; van Es, D.S.; de Jong, K.P.; Bitter, J.H.

    2013-01-01

    Carbon nanofibers (CNFs) were functionalized with aryl sulfonic acid groups using in situ diazonium coupling. The use of diazonium coupling yielded an acidic carbon material, in which the introduced acidic groups are readily accessible to the triglyceride substrate. The material is an efficient

  2. Functionalized carbon nanofibers as solid-acid catalysts for transesterification

    NARCIS (Netherlands)

    Stellwagen, D.R.; Klis, van der F.; Es, van D.S.; Jong, de K.P.; Bitter, J.H.

    2013-01-01

    Carbon nanofibers (CNFs) were functionalized with aryl sulfonic acid groups using in situ diazonium coupling. The use of diazonium coupling yielded an acidic carbon material, in which the introduced acidic groups are readily accessible to the triglyceride substrate. The material is an efficient

  3. Preparation of Pt–Ru bimetallic catalyst supported on carbon

    Indian Academy of Sciences (India)

    The template carbonization of polyphenyl acetylene yields hollow, uniform cylindrical carbon nanotubes with outer diameter almost equal to pore diameter of the template used. High resolution transmission electron microscopic investigation reveals that Pt–Ru nanoparticles are highly dispersed inside the tube with an ...

  4. Activity of molybdenum-containing oxide catalysts in the reaction of ethane oxidation

    International Nuclear Information System (INIS)

    Konovalov, V.I.; Ehpova, T.I.; Shchukin, V.P.; Averbukh, A.Ya.

    1977-01-01

    Investigation results concerning the catalytic activity of molybdenum-containing catalysts in ethane oxidation reaction are presented. It has been found that the greatest activity in the temperature range from 450 to 600 deg C is exhibited by cobalt-molybdenum catalyst; at 600 deg C bismuth-molybdenum catalyst is the most active. Nickel-molybdenum catalyst is selective and active with respect to ethylene. Iron- and manganese-molybdenum catalysts do not show high ethane oxidation rates and their selectivity is insignificant

  5. Production of carbon nanotubes: Chemical vapor deposition synthesis from liquefied petroleum gas over Fe-Co-Mo tri-metallic catalyst supported on MgO

    Energy Technology Data Exchange (ETDEWEB)

    Setyopratomo, P., E-mail: puguh-sptm@yahoo.com; Wulan, Praswasti P. D. K., E-mail: wulanmakmur@gmail.com; Sudibandriyo, M., E-mail: msudib@che.ui.ac.id [Chemical Engineering Department, University of Indonesia, Depok Campus, Depok 16424 (Indonesia)

    2016-06-03

    Carbon nanotubes were produced by chemical vapor deposition method to meet the specifications for hydrogen storage. So far, the various catalyst had been studied outlining their activities, performances, and efficiencies. In this work, tri-metallic catalyst consist of Fe-Co-Mo supported on MgO was used. The catalyst was prepared by wet-impregnation method. Liquefied Petroleum Gas (LPG) was used as carbon source. The synthesis was conducted in atmospheric fixed bed reactor at reaction temperature range 750 – 850 °C for 30 minutes. The impregnation method applied in this study successfully deposed metal component on the MgO support surface. It found that the deposited metal components might partially replace Mg(OH){sub 2} or MgO molecules in their crystal lattice. Compare to the original MgO powder; it was significant increases in pore volume and surface area has occurred during catalyst preparation stages. The size of obtained carbon nanotubes is ranging from about 10.83 nm OD/4.09 nm ID up to 21.84 nm OD/6.51 nm ID, which means that multiwall carbon nanotubes were formed during the synthesis. Yield as much as 2.35 g.CNT/g.catalyst was obtained during 30 minutes synthesis and correspond to carbon nanotubes growth rate of 0.2 μm/min. The BET surface area of the obtained carbon nanotubes is 181.13 m{sup 2}/g and around 50 % of which is contributed by mesopores. Micropore with half pore width less than 1 nm contribute about 10% volume of total micro and mesopores volume of the carbon nanotubes. The existence of these micropores is very important to increase the hydrogen storage capacity of the carbon nanotubes.

  6. Gold Nanoparticles on Polymer-Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO2.

    Science.gov (United States)

    Jhong, Huei-Ru Molly; Tornow, Claire E; Kim, Chaerin; Verma, Sumit; Oberst, Justin L; Anderson, Paul S; Gewirth, Andrew A; Fujigaya, Tsuyohiko; Nakashima, Naotoshi; Kenis, Paul J A

    2017-11-17

    Multiple approaches will be needed to reduce the atmospheric CO 2 levels, which have been linked to the undesirable effects of global climate change. The electroreduction of CO 2 driven by renewable energy is one approach to reduce CO 2 emissions while producing chemical building blocks, but current electrocatalysts exhibit low activity and selectivity. Here, we report the structural and electrochemical characterization of a promising catalyst for the electroreduction of CO 2 to CO: Au nanoparticles supported on polymer-wrapped multiwall carbon nanotubes. This catalyst exhibits high selectivity for CO over H 2 : 80-92 % CO, as well as high activity: partial current density for CO as high as 160 mA cm -2 . The observed high activity, originating from a high electrochemically active surface area (23 m 2  g -1 Au), in combination with the low loading (0.17 mg cm -2 ) of the highly dispersed Au nanoparticles underscores the promise of this catalyst for efficient electroreduction of CO 2 . © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. Synthesis and field emission properties of carbon nanotubes grown in ethanol flame based on a photoresist-assisted catalyst annealing process

    International Nuclear Information System (INIS)

    Yang Xiaoxia; Fang Guojia; Liu Nishuang; Wang Chong; Zheng Qiao; Zhou Hai; Zhao Dongshan; Long Hao; Liu Yuping; Zhao Xingzhong

    2009-01-01

    Carbon nanotubes (CNTs) have been grown directly on a Si substrate without a diffusion barrier in ethanol diffusion flame using Ni as the catalyst after a photoresist-assisted catalyst annealing process. The growth mechanism of as-synthesized CNTs is confirmed by scanning electron microscopy, high resolution transmission-electron microscopy and energy-dispersive spectroscopy. The photoresist is the key for the formation of active catalyst particles during annealing process, which then result in the growth of CNTs. The catalyst annealing temperature has been found to affect the morphologies and field electron emission properties of CNTs significantly. The field emission properties of as-grown CNTs are investigated with a diode structure and the obtained CNTs exhibit enhanced characteristics. This technique will be applicable to a low-cost fabrication process of electron-emitter arrays.

  8. Effect of W on activity of Pt-Ru/C catalyst for methanol electrooxidation in acidic medium

    International Nuclear Information System (INIS)

    Wang Zhenbo; Zuo Pengjian; Yin Geping

    2009-01-01

    The effect of W on the activity of Pt-Ru/C catalyst was investigated. The Pt-Ru-W/C and Pt-Ru/C-TR catalysts were prepared by thermal reduction method. Comparison was made to a homemade Pt-Ru/C-CR catalyst prepared by chemical reduction. Their performances were tested by using a glassy carbon thin film electrode through cyclic voltammetric and chronoamperometric curves. The particle size, structure, composition, and surface state of homemade catalyst were determined by means of X-ray diffraction (XRD), energy dispersive analysis of X-ray (EDAX), transmission electron microscopy (TEM), and X-ray photoelectron spectrometry (XPS). The result of XRD analysis shows that the homemade ternary catalyst exhibits face-centered cubic structure and has smaller lattice parameter than Pt-alone and homemade Pt-Ru/C catalysts. The particle size of Pt-Ru-W/C catalyst is relatively large of 6.5 nm. Its electrochemically active specific area is 20 m 2 g -1 less than that of Pt-Ru/C-CR, and much twice as big as that of Pt-Ru/C-TR. But, XPS analysis shows that the addition of W changes the surface state of Pt components in the alloy and can clean Pt surface active sites which are adsorbed by hydrogen. The electrocatalytic activity and tolerance performance to CO ads of Pt-Ru-W/C catalyst for methanol electrooxidation is the best due to the promoting function of W in comparison with homemade Pt-Ru/C ones.

  9. Characterization of Cu/CeO2/Al2O3 catalysts by temperature programmed reduction and activity for CO oxidation

    International Nuclear Information System (INIS)

    Cataluna, Renato; Baibich, Ione M.; Dallago, R.M.; Picinini, C.; Martinez-Arias, A.; Soria, J.

    2001-01-01

    The kinetic parameters for the CO oxidation reaction using copper/alumina-modified ceria as catalysts were determined. The catalysts with different concentrations of the metals were prepared using impregnation methods. In addition, the reduction-oxidation behaviour of the catalysts were investigated by temperature-programmed reduction. The activity results show that the mechanism for CO oxidation is bifunctional: oxygen is activated on the anionic vacancies of ceria surface, while carbon monoxide is adsorbed preferentially on the higher oxidation copper site. Therefore, the reaction occurs on the interfacial active centers. Temperatures-programmed Reduction patterns show a higher dispersion when cerium oxide is present. (author)

  10. Dehydrogenation of Isobutane with Carbon Dioxide over SBA-15-Supported Vanadium Oxide Catalysts

    Directory of Open Access Journals (Sweden)

    Chunling Wei

    2016-10-01

    Full Text Available A series of vanadia catalysts supported on SBA-15 (V/SBA with a vanadia (V content ranging from 1% to 11% were prepared by an incipient wetness method. Their catalytic behavior in the dehydrogenation of isobutane to isobutene with CO2 was examined. The catalysts were characterized by N2 adsorption, X-ray diffraction (XRD, scanning electron microscopy (SEM, Raman spectroscopy, and temperature-programmed reduction (TPR. It was found that these catalysts were effective for the dehydrogenation reaction, and the catalytic activity is correlated with the amount of dispersed vanadium species on the SBA-15 support. The 7% V/SBA catalyst shows the highest activity, which gives 40.8% isobutane conversion and 84.8% isobutene selectivity. The SBA-15-supported vanadia exhibits higher isobutane conversion and isobutene selectivity than the MCM-41-supported one.

  11. Flame synthesis of carbon nano onions using liquefied petroleum gas without catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Dhand, Vivek, E-mail: vivekdhand2012@gmail.com [Centre for Knowledge Management of Nanoscience and Technology, 12-5-32/8, Vijayapuri Colony, Tarnaka, Secunderabad-500 017, A.P (India); Prasad, J. Sarada; Rao, M. Venkateswara [Centre for Environment, Institute of Science and Technology, Jawaharlal Nehru Technological University, Kukatpally, Hyderabad 500 085 (India); Bharadwaj, S. [Department of Physics, CVR College of Engineering and Osmania University, Hyderabad 501510, A.P (India); Anjaneyulu, Y. [TLGVRC, Jackson State University, JSU Box 18739, Jackson, MS 39217-0939 (United States); Jain, Pawan Kumar [International Advanced Research Centre for Powder Metallurgy and New Materials (ARCI), Balapur PO, Hyderabad 500005, Andhra Pradesh (India)

    2013-03-01

    Densely agglomerated, high specific surface area carbon nano onions with diameter of 30-40 nm have been synthesized. Liquefied petroleum gas and air mixtures produced carbon nano onions in diffusion flames without catalyst. The optimized oxidant to fuel ratio which produces carbon nano onions has been found to be 0.1 slpm/slpm. The experiment yielded 70% pure carbon nano onions with a rate of 5 g/h. X-ray diffraction, high-resolution electron microscopy and Raman spectrum reveal the densely packed sp{sup 2} hybridized carbon with (002) semi-crystalline hexagonal graphite reflection. The carbon nano onions are thermally stable up to 600 Degree-Sign C. - Highlights: Black-Right-Pointing-Pointer Flame synthesized carbon nano onions with 30-40 nm diameters. Black-Right-Pointing-Pointer LPG/air, diffusion type flame used in absence of catalyst to produce nano onions. Black-Right-Pointing-Pointer Carbon nano onion production rate is 5 g/hr and with 70% purity.

  12. A combined in situ XAS-XRPD-Raman study of Fischer-Tropsch synthesis over a carbon supported Co catalyst

    DEFF Research Database (Denmark)

    Tsakoumis, Nikolaos E.; Dehghan, Roya; Johnsen, Rune

    2013-01-01

    A cobalt based Fischer-Tropsch synthesis (FTS) catalyst, supported on a carbon nanofibers/carbon felt composite (Co/CNF/CF) was studied in situ at realistic conditions. The catalyst was monitored by Xray absorption spectroscopy (XAS), high-resolution X-ray powder diffraction (HR-XRPD) and Raman...... spectroscopy, while changes in the gas phase were observed by mass spectrometry (MS). Transmission electron microscopy (TEM) was also applied to characterise the catalyst. The catalyst has a bimodal particle size distribution and exhibits a high deactivation rate. During the in situ study the catalyst appears...... to reduce further at the induction period of FTS, while crystallite growth is been detected in the same period. At steady state FTS the amount of metallic Co is constant. A change in the volumetric flow towards higher conversions did not affect the degree of reduction or the crystallite size of the catalyst...

  13. Activation of peroxymonosulfate by graphitic carbon nitride loaded on activated carbon for organic pollutants degradation

    Energy Technology Data Exchange (ETDEWEB)

    Wei, Mingyu; Gao, Long; Li, Jun [School of Environmental Engineering, Wuhan Textile University, Wuhan 430073 (China); Fang, Jia [School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430073 (China); Cai, Wenxuan [School of Environmental Engineering, Wuhan Textile University, Wuhan 430073 (China); Li, Xiaoxia [School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430073 (China); Xu, Aihua, E-mail: xahspinel@sina.com [School of Environmental Engineering, Wuhan Textile University, Wuhan 430073 (China); Engineering Research Center for Clean Production of Textile Dyeing and Printing, Ministry of Education, Wuhan 430073 (China)

    2016-10-05

    Highlights: • Supported g-C{sub 3}N{sub 4} on AC catalysts with different loadings were prepared. • The metal free catalysts exhibited high efficiency for dyes degradation with PMS. • The catalyst presented a long-term stability for multiple runs. • The C=O groups played a key role in the oxidation process. - Abstract: Graphitic carbon nitride supported on activated carbon (g-C{sub 3}N{sub 4}/AC) was prepared through an in situ thermal approach and used as a metal free catalyst for pollutants degradation in the presence of peroxymonosulfate (PMS) without light irradiation. It was found that g-C{sub 3}N{sub 4} was highly dispersed on the surface of AC with the increase of surface area and the exposition of more edges and defects. The much easier oxidation of C species in g-C{sub 3}N{sub 4} to C=O was also observed from XPS spectra. Acid Orange 7 (AO7) and other organic pollutants could be completely degraded by the g-C{sub 3}N{sub 4}/AC catalyst within 20 min with PMS, while g-C{sub 3}N{sub 4}+PMS and AC+PMS showed no significant activity for the reaction. The performance of the catalyst was significantly influenced by the amount of g-C{sub 3}N{sub 4} loaded on AC; but was nearly not affected by the initial solution pH and reaction temperature. In addition, the catalysts presented good stability. A nonradical mechanism accompanied by radical generation (HO· and SO{sub 4}·{sup −}) in AO7 oxidation was proposed in the system. The C=O groups play a key role in the process; while the exposure of more N-(C){sub 3} group can further increase its electron density and basicity. This study can contribute to the development of green materials for sustainable remediation of aqueous organic pollutants.

  14. Synthesis of a carbon-coated NiO/MgO core/shell nanocomposite as a Pd electro-catalyst support for ethanol oxidation

    International Nuclear Information System (INIS)

    Mahendiran, C.; Maiyalagan, T.; Scott, K.; Gedanken, A.

    2011-01-01

    Highlights: → Carbon coated on NiO/MgO in a core/shell nanostructure is synthesized by RAPET. → The carbon-coated NiO/MgO is supported by Pd. → The electrocatalytic properties of the Pd/(NiO/MgO-C) catalyst for ethanol oxidation studied. - Abstract: Carbon coated on NiO/MgO in a core/shell nanostructure was synthesized by the single-step RAPET (reaction under autogenic pressure at elevated temperatures) technique, and the obtained formation mechanism of the core/shell nanocomposite was presented. The carbon-coated NiO/MgO and its supported Pd catalyst, Pd/(NiO/MgO-C), were characterized by SEM, HR-TEM, XRD and cyclic voltammetry. The X-ray diffraction patterns confirmed the face-centered cubic crystal structure of NiO/MgO. Raman spectroscopy measurements provided structural evidence for the formation of a NiO/MgO composite and the nature of the coated carbon shell. The high-resolution transmission electron microscopy images showed the core and shell morphologies individually. The electrocatalytic properties of the Pd/(NiO/MgO-C) catalyst for ethanol oxidation were investigated in an alkaline solution. The results indicated that the prepared Pd-NiO/MgO-C catalyst has excellent electrocatalytic activity and stability.

  15. Hydrogenation active sites of unsupported molybdenum sulfide catalysts for hydroprocessing heavy oils

    Energy Technology Data Exchange (ETDEWEB)

    Iwata, Y.; Araki, Y.; Honna, K. [Tsukuba-branch, Advanced Catalyst Research Laboratory, Petroleum Energy Center, 1-1 Higashi, Tsukuba, 305-8565 Ibaraki (Japan); Miki, Y.; Sato, K.; Shimada, H. [National Institute of Materials and Chemical Research, 1-1 Higashi, Tsukuba, 305-8565 Ibaraki (Japan)

    2001-02-20

    The purpose of the present study was to elucidate the nature of the hydrogenation active sites on unsupported molybdenum sulfide catalysts, aimed at the improvement of the catalysts for the slurry processes. The number of hydrogenation active sites was found to relate to the 'inflection' on the basal plane of the catalyst particles. The comparison of the catalytic activity to that of an oil-soluble catalyst in the hydroprocessing of heavy oils suggests that the performance of the oil-soluble catalyst was near the maximum, unless another component such as Ni or Co was incorporated.

  16. Synthesis, Characterization and Application of A Novel Carbon Bridged Half-metallocene Chromium Catalyst for Methyl Methacrylate Polymerization

    Institute of Scientific and Technical Information of China (English)

    CHENG Zhengzai; GONG Kai; WANG Yang; ZHOU Xue; ZHANG Weixing; LI Yin; SUN Junquan; LI Wenbing

    2014-01-01

    A new carbon bridged cyclopentadienyl chromium complex of the type [(C5H4)C(CH3)2 CH2(C5H4N)]CrCl2 was prepared by treatment of CrCl3•(THF)3 in THF solution with the lithium salt of ligand containing cyclopentadienyl and pyridyl groups. The chromium complex was characterized by 1H NMR and elemental analysis(EA), and the crystal structure was determined by X-ray diffraction analysis. Activated by Al(i-Bu)3, the chromium complex displayed a very high activity for methyl methacrylate (MMA) polymerization. After 24 hours,more than 95.5%MMA was converted to polymethyl methacrylate (PMMA) with a viscosity average molecular weight (Wη) of 416000 g•mol-1 at 60℃for MMA/Al(i-Bu)3/chromium catalyst molar ratio of up to 2000:20:1. Effects of temperature, molar ratios of MMA/catalyst and catalyst/cocatalyst on the polymerization have been studied. The high conversion of MMA and high molecular weight of PMMA with narrow molecular weight distribution is caused by the unique stable active site formed by the new chromium complex and aluminum cocatalyst.

  17. Formation of Platinum Catalyst on Carbon Black Using an In‐Liquid Plasma Method for Fuel Cells

    Directory of Open Access Journals (Sweden)

    Yoshiyuki Show

    2017-01-01

    Full Text Available Platinum (Pt catalyst was formed on the surface of carbon black using an in‐liquid plasma method. The formed Pt catalyst showed the average particle size of 4.1 nm. This Pt catalyst was applied to a polymer electrolyte membrane fuel cell (PEMFC. The PEMFC showed an open voltage of 0.85 V and a maximum output power density of 216 mW/cm2.

  18. Hydrogen production by dry reforming of methane with carbon dioxide in one-dimensional nickel-based catalysts; Produccion de hidrogeno mediante el reformado seco de metano con dioxido de carbono en catalizadores unidimensionales a base de niquel

    Energy Technology Data Exchange (ETDEWEB)

    Lopez U, A. C.

    2016-07-01

    The main objective of this thesis is development of nickel catalysts supported over 1D matrix of cerium oxide, to be used in dry reforming methane reaction with carbon dioxide for hydrogen production. The catalysts were characterized by: Temperature Programmed Reduction (TPR), Scanning Electronic Microscopy (Sem), Surface Area (Bet method) an X Ray Diffraction (XRD). The TPR technique allowed to define reduction temperature of the active phase in the catalyst, Sem technique showed that the CeO{sub 2} matrix had a nano rod morphology. XRD allowed to identify the crystalline phases of the catalysts. Finally, the catalysts were tested in the dry reforming methane reaction, high catalytic activity and hydrogen production were performed at 700 degrees Celsius and the catalyst with 30 wt.% of nickel. (Author)

  19. Fluorine-doped carbon nanotubes as an efficient metal-free catalyst for destruction of organic pollutants in catalytic ozonation.

    Science.gov (United States)

    Wang, Jing; Chen, Shuo; Quan, Xie; Yu, Hongtao

    2018-01-01

    Metal-free carbon materials have been presented to be potential alternatives to metal-based catalysts for heterogeneous catalytic ozonation, yet the catalytic performance still needs to be enhanced. Doping carbon with non-metallic heteroatoms (e.g., N, B, and F) could alter the electronic structure and electrochemical properties of original carbon materials, has been considered to be an effective method for improving the catalytic activity of carbon materials. Herein, fluorine-doped carbon nanotubes (F-CNTs) were synthesized via a facile method and characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The as-synthesized F-CNTs exhibited notably enhanced catalytic activity towards catalytic ozonation for the degradation of organic pollutants. The oxalic acid removal efficiency of optimized F-CNTs was approximately two times as much as that of pristine CNTs, and even exceeded those of four conventional metal-based catalysts (ZnO, Al 2 O 3 , Fe 2 O 3 , and MnO 2 ). The XPS and Raman studies confirmed that the covalent CF bonds were formed at the sp 3 C sites instead of sp 2 C sites on CNTs, not only resulting in high positive charge density of C atoms adjacent to F atoms, but remaining the delocalized π-system with intact carbon structure of F-CNTs, which then favored the conversion of ozone molecules (O 3 ) into reactive oxygen species (ROS) and contributed to the high oxalic acid removal efficiency. Furthermore, electron spin resonance (ESR) studies revealed that superoxide radicals (O 2 - ) and singlet oxygen ( 1 O 2 ) might be the dominant ROS that responsible for the degradation of oxalic acid in these catalytic systems. Copyright © 2017 Elsevier Ltd. All rights reserved.

  20. Carbon nanostructures as catalyst support for polymer electrolyte membrane fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Natarajan, S.K.; Hamelin, J. [Quebec Univ., Trois Rivieres, PQ (Canada). Inst. de recherche sur l' hydrogene

    2008-07-01

    This paper reported on a study that investigated potential alternatives to Vulcan XC-72 as a catalyst supports for polymer electrolyte membrane fuel cells (PEMFCs). These included carbon nanostructures (CNS) prepared by high energy ball milling of graphite and transition metal catalysts, followed by heat treatment. Among the key factors discussed were the graphitic content, high surface area, microporous structure, good electrical conductivity and the ability of the material to attach functional groups. Some graphic results supporting the usage of CNS as catalyst support for PEMFCs were presented. Upon chemical oxidation, surface functional groups such as carbonyl, carboxyl, and hydroxyl were populated on the surface of CNS. Nanosized platinum particles with particle size distribution between 3 nm and 5 nm were reduced on the functionalized sites of CNS in a colloidal medium. The paper also presented cyclic voltammograms, XPS, HRTEM and PSD results. 3 refs.

  1. Wet catalyst-support films for production of vertically aligned carbon nanotubes.

    Science.gov (United States)

    Alvarez, Noe T; Hamilton, Christopher E; Pint, Cary L; Orbaek, Alvin; Yao, Jun; Frosinini, Aldo L; Barron, Andrew R; Tour, James M; Hauge, Robert H

    2010-07-01

    A procedure for vertically aligned carbon nanotube (VA-CNT) production has been developed through liquid-phase deposition of alumoxanes (aluminum oxide hydroxides, boehmite) as a catalyst support. Through a simple spin-coating of alumoxane nanoparticles, uniform centimer-square thin film surfaces were coated and used as supports for subsequent deposition of metal catalyst. Uniform VA-CNTs are observed to grow from this film following deposition of both conventional evaporated Fe catalyst, as well as premade Fe nanoparticles drop-dried from the liquid phase. The quality and uniformity of the VA-CNTs are comparable to growth from conventional evaporated layers of Al(2)O(3). The combined use of alumoxane and Fe nanoparticles to coat surfaces represents an inexpensive and scalable approach to large-scale VA-CNT production that makes chemical vapor deposition significantly more competitive when compared to other CNT production techniques.

  2. Catalysts for the production of hydrocarbons from carbon monoxide and water

    Science.gov (United States)

    Sapienza, R.S.; Slegeir, W.A.; Goldberg, R.I.

    1985-11-06

    A method of converting low H/sub 2//CO ratio syngas to carbonaceous products comprising reacting the syngas with water or steam at 200 to 350/sup 0/C in the presence of a metal catalyst supported on zinc oxide. Hydrocarbons are produced with a catalyst selected from cobalt, nickel or ruthenium and alcohols are produced with a catalyst selected from palladium, platinum, ruthenium or copper on the zinc oxide support. The ratio of the reactants are such that for alcohols and saturated hydrocarbons: (2n + 1) greater than or equal to x greater than or equal to O and for olefinic hydrocarbons: 2n greater than or equal to x greater than or equal to O where n is the number of carbon atoms in the product and x is the molar amount of water in the reaction mixture.

  3. Catalyst effects of fabrication of carbon nanotubes synthesized by chemical vapor deposition

    International Nuclear Information System (INIS)

    Tian, F.; Li, H.P.; Zhao, N.Q.; He, C.N.

    2009-01-01

    Catalytic effects of the fabrication of carbon nanotubes (CNTs) by chemical vapor deposition of methane were investigated by thermogravimetric analysis. More specifically, the total yield and thermal stability characteristics of the product were examined with respect to physicochemical characteristics of the catalyst. Three kinds of Ni/Al catalysts with 5 wt%, 10 wt% and 15 wt% Ni, respectively were employed to synthesize CNTs. It was determined that an optimal Ni content of the catalyst resulted in maximum yield and most stable product. With increasing the Ni content, the CNT yield increased but they became less stable during heat treatment in air. According to transmission electron microscopy observations, the defect sites along the walls and at the ends of the raw CNTs facilitated the thermal oxidative destruction of the CNTs.

  4. Growth of uniform thin-walled carbon nanotubes with spin-coated Fe catalyst and the correlation between the pre-growth catalyst size and the nanotube diameter

    International Nuclear Information System (INIS)

    Seah, Choon-Ming; Chai, Siang-Piao; Ichikawa, Satoshi; Mohamed, Abdul Rahman

    2013-01-01

    Single-walled carbon nanotubes (CNTs) and double-walled CNTs with a selectivity of 93 % were obtained by means of the novel homemade iron catalysts which were spin coated on silicon wafer. The average diameters of the iron particles prepared from the colloidal solutions containing 30, 40, 50, 60, and 70 mmol/L of iron nitrate were 8.2, 5.1, 20.8, 32.2, and 34.7 nm, respectively, and growing thin-walled CNTs with the average diameters of 4.1, 2.2, 9.2, 11.1, and 18.1 nm, respectively. The diameters of the CNTs were correlated with the geometric sizes of the pre-growth catalyst particles. Thin-walled CNTs were found to have a catalyst mean diameter-to-CNT average diameter ratio of 2.31. Iron carbide was formed after the growth of CNTs, and it is believed that during the growth of CNTs, carbon source decomposed and deposited on the surface of catalyst, followed by the diffusion of surface carbon into the iron catalyst particles, resulting in carbon supersaturation state before the growth of CNTs.

  5. Patched bimetallic surfaces are active catalysts for ammonia decomposition.

    Science.gov (United States)

    Guo, Wei; Vlachos, Dionisios G

    2015-10-07

    Ammonia decomposition is often used as an archetypical reaction for predicting new catalytic materials and understanding the very reason of why some reactions are sensitive on material's structure. Core-shell or surface-segregated bimetallic nanoparticles expose outstanding activity for many heterogeneously catalysed reactions but the reasons remain elusive owing to the difficulties in experimentally characterizing active sites. Here by performing multiscale simulations in ammonia decomposition on various nickel loadings on platinum (111), we show that the very high activity of core-shell structures requires patches of the guest metal to create and sustain dual active sites: nickel terraces catalyse N-H bond breaking and nickel edge sites drive atomic nitrogen association. The structure sensitivity on these active catalysts depends profoundly on reaction conditions due to kinetically competing relevant elementary reaction steps. We expose a remarkable difference in active sites between transient and steady-state studies and provide insights into optimal material design.

  6. Continuous synthesis of methanol: heterogeneous hydrogenation of ethylene carbonate over Cu/HMS catalysts in a fixed bed reactor system.

    Science.gov (United States)

    Chen, Xi; Cui, Yuanyuan; Wen, Chao; Wang, Bin; Dai, Wei-Lin

    2015-09-18

    Continuous fixed-bed catalytic hydrogenation of ethylene carbonate (EC) to methanol and ethylene glycol (EG), an emerging synthetic process of methanol via indirect conversion of CO2, was successfully performed over Cu/HMS catalysts prepared by the ammonia evaporation (AE) method. The catalysts possessed superb performance with a conversion of 100% and a selectivity to methanol of 74%.

  7. 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.

  8. New sulfide catalysts for the hydroliquefaction of coal

    NARCIS (Netherlands)

    Vissers, J.P.R.; Oers, van E.M.; Beer, de V.H.J.; Prins, R.

    1987-01-01

    Possibilities for the preparation of new metal sulfide catalyst systems based on carbon carriers having favourable textural and surface properties have been explored, and attention has been given to the characterization (structure) and evaluation (hydrosulfurization activity) of these catalysts. Two

  9. PtRu catalysts supported on heteropolyacid and chitosan functionalized carbon nanotubes for methanol oxidation reaction of fuel cells.

    Science.gov (United States)

    Cui, Zhiming; Li, Chang Ming; Jiang, San Ping

    2011-09-28

    A simple self-assembly approach has been developed to functionalize carbon nanotubes (CNTs) with chitosan (CS) and heteropolyacids (HPAs) of phosphomolybdic acid (H(3)PMo(12)O(40), HPMo) and phosphotungstic acid (H(3)PW(12)O(40), HPW). The non-covalent functionalization method, which introduces homogenous surface functional groups with no detrimental effect on graphene structures of CNTs, can be carried out at room temperature without the use of corrosive acids. The PtRu nanoparticles supported on HPAs-CS-CNTs have a uniform distribution and much smaller size as compared to those of the PtRu nanoparticles supported on conventional acid treated CNTs (PtRu/AO-CNTs). The onset and peak potentials for CO(ad) oxidation on PtRu/HPAs-CS-CNTs catalysts are more negative than those on PtRu/AO-CNTs, indicating that HPAs facilitate the electro-oxidation of CO. The PtRu/HPMo-CS-CNTs catalyst has a higher electrocatalytic activity for methanol oxidation and higher tolerance toward CO poisoning than PtRu/HPW-CS-CNTs. The better electrocatalytic enhancement of HPMo on the PtRu/HPAs-CS-CNTs catalyst is most likely related to the fact that molybdenum-containing HPAs such as HPMo have more labile terminal oxygen to provide additional active oxygen sites while accelerating the CO and methanol oxidation in a similar way to that of Ru in the PtRu binary alloy system.

  10. Photocatalytic carbon dioxide reduction with rhodium-based catalysts in solution and heterogenized within metal-organic frameworks.

    Science.gov (United States)

    Chambers, Matthew B; Wang, Xia; Elgrishi, Noémie; Hendon, Christopher H; Walsh, Aron; Bonnefoy, Jonathan; Canivet, Jérôme; Quadrelli, Elsje Alessandra; Farrusseng, David; Mellot-Draznieks, Caroline; Fontecave, Marc

    2015-02-01

    The first photosensitization of a rhodium-based catalytic system for CO2 reduction is reported, with formate as the sole carbon-containing product. Formate has wide industrial applications and is seen as valuable within fuel cell technologies as well as an interesting H2 -storage compound. Heterogenization of molecular rhodium catalysts is accomplished via the synthesis, post-synthetic linker exchange, and characterization of a new metal-organic framework (MOF) Cp*Rh@UiO-67. While the catalytic activities of the homogeneous and heterogeneous systems are found to be comparable, the MOF-based system is more stable and selective. Furthermore it can be recycled without loss of activity. For formate production, an optimal catalyst loading of ∼10 % molar Rh incorporation is determined. Increased incorporation of rhodium catalyst favors thermal decomposition of formate into H2 . There is no precedent for a MOF catalyzing the latter reaction so far. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. 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

  12. Highly Loaded Carbon Black Supported Pt Catalysts for Fuel Cells

    Czech Academy of Sciences Publication Activity Database

    Kaluža, Luděk; Larsen, M.J.; Zdražil, Miroslav; Gulková, Daniela; Vít, Zdeněk; Šolcová, Olga; Soukup, Karel; Koštejn, Martin; Bonde, J.L.; Maixnerová, Lucie; Odgaard, M.

    2015-01-01

    Roč. 256, NOV 1 (2015), s. 375-383 ISSN 0920-5861 R&D Projects: GA MŠk(CZ) 7HX13003 EU Projects: European Commission(XE) 303466 - IMMEDIATE Institutional support: RVO:67985858 Keywords : carbon black * fuell cell * electrocatalyst Subject RIV: CI - Industrial Chemistry , Chemical Engineering Impact factor: 4.312, year: 2015

  13. Performance of carbon nanofiber supported Pd-Ni catalysts for electro-oxidation of ethanol in alkaline medium

    Science.gov (United States)

    Maiyalagan, T.; Scott, Keith

    Carbon nanofibers (CNF) supported Pd-Ni nanoparticles have been prepared by chemical reduction with NaBH 4 as a reducing agent. The Pd-Ni/CNF catalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and electrochemical voltammetry analysis. TEM showed that the Pd-Ni particles were quite uniformly distributed on the surface of the carbon nanofiber with an average particle size of 4.0 nm. The electro-catalytic activity of the Pd-Ni/CNF for oxidation of ethanol was examined by cyclic voltammetry (CV). The onset potential was 200 mV lower and the peak current density four times higher for ethanol oxidation for Pd-Ni/CNF compared to that for Pd/C. The effect of an increase in temperature from 20 to 60 °C had a great effect on increasing the ethanol oxidation activity.

  14. Performance of carbon nanofiber supported Pd-Ni catalysts for electro-oxidation of ethanol in alkaline medium

    Energy Technology Data Exchange (ETDEWEB)

    Maiyalagan, T.; Scott, Keith [School of Chemical Engineering and Advanced Materials, University of Newcastle upon Tyne, Newcastle upon Tyne NE1 7RU (United Kingdom)

    2010-08-15

    Carbon nanofibers (CNF) supported Pd-Ni nanoparticles have been prepared by chemical reduction with NaBH{sub 4} as a reducing agent. The Pd-Ni/CNF catalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and electrochemical voltammetry analysis. TEM showed that the Pd-Ni particles were quite uniformly distributed on the surface of the carbon nanofiber with an average particle size of 4.0 nm. The electro-catalytic activity of the Pd-Ni/CNF for oxidation of ethanol was examined by cyclic voltammetry (CV). The onset potential was 200 mV lower and the peak current density four times higher for ethanol oxidation for Pd-Ni/CNF compared to that for Pd/C. The effect of an increase in temperature from 20 to 60 C had a great effect on increasing the ethanol oxidation activity. (author)

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

    International Nuclear Information System (INIS)

    Naeem, R.; Ahmed, R.; Ansari, M.S.

    2013-01-01

    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

  16. Structural and electrochemical characterization of carbon supported Pt-Pr catalysts for direct ethanol fuel cells prepared using a modified formic acid method in a CO atmosphere.

    Science.gov (United States)

    Corradini, Patricia Gon; Antolini, Ermete; Perez, Joelma

    2013-07-28

    Pt-Pr/C electrocatalysts were prepared using a modified formic acid method, and their activity for carbon monoxide and ethanol oxidation was compared to Pt/C. No appreciable alloy formation was detected by XRD analysis. By TEM measurements it was found that Pt particle size increases with an increasing Pr content in the catalysts and with decreasing metal precursor addition time. XPS measurements indicated Pt segregation on the catalyst surface and the presence of Pr2O3 and PrO2 oxides. The addition of Pr increased the electro-catalytic activity of Pt for both CO and CH3CH2OH oxidation. The enhanced activity of Pt-Pr/C catalysts was ascribed to both an electronic effect, caused by the presence of Pr2O3, and the bi-functional mechanism, caused by the presence of PrO2.

  17. On factors controlling activity of submonolayer bimetallic catalysts: Nitrogen desorption

    Energy Technology Data Exchange (ETDEWEB)

    Guo, Wei; Vlachos, Dionisios G., E-mail: vlachos@udel.edu [Center for Catalytic Science and Technology, Catalysis Center for Energy Innovation, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, Delaware 19716 (United States)

    2014-01-07

    We model N{sub 2} desorption on submonolayer bimetallic surfaces consisting of Co clusters on Pt(111) via first-principles density functional theory-based kinetic Monte Carlo simulations. We find that submonolayer structures are essential to rationalize the high activity of these bimetallics in ammonia decomposition. We show that the N{sub 2} desorption temperature on Co/Pt(111) is about 100 K higher than that on Ni/Pt(111), despite Co/Pt(111) binding N weaker at low N coverages. Co/Pt(111) has substantially different lateral interactions than single metals and Ni/Pt. The lateral interactions are rationalized with the d-band center theory. The activity of bimetallic catalysts is the result of heterogeneity of binding energies and reaction barriers among sites, and the most active site can differ on various bimetallics. Our results are in excellent agreement with experimental data and demonstrate for the first time that the zero-coverage descriptor, used until now, for catalyst activity is inadequate due not only to lacking lateral interactions but importantly to presence of multiple sites and a complex interplay of thermodynamics (binding energies, occupation) and kinetics (association barriers) on those sites.

  18. Visible-Light-Responsive Catalyst Development for Volatile Organic Carbon Remediation Project

    Science.gov (United States)

    Zeitlin, Nancy; Hintze, Paul E.; Coutts, Janelle

    2015-01-01

    Photocatalysis is a process in which light energy is used to 'activate' oxidation/reduction reactions. Unmodified titanium dioxide (TiO2), a common photocatalyst, requires high-energy UV light for activation due to its large band gap (3.2 eV). Modification of TiO2 can reduce this band gap, leading to visible-light-responsive (VLR) photocatalysts. These catalysts can utilize solar and/or visible wavelength LED lamps as an activation source, replacing mercury-containing UV lamps, to create a "greener," more energy-efficient means for air and water revitalization. Recently, KSC developed several VLR catalysts that, on preliminary evaluation, possessed high catalytic activity within the visible spectrum; these samples out-performed existing commercial VLR catalysts.

  19. Enhanced activity and durability of platinum anode catalyst by the modification of cobalt phosphide for direct methanol fuel cells

    International Nuclear Information System (INIS)

    Li, Xiang; Wang, Hongjuan; Yu, Hao; Liu, Ziwu; Wang, Haihui; Peng, Feng

    2015-01-01

    Graphical abstract: A novel Pt/CoP/CNTs electrocatalyst with has been designed and prepared, which exhibits high activity and stability for methanol oxidation reaction. - Highlights: • Pt-cobalt phosphide catalyst supported on carbon nanotubes (Pt/CoP/CNTs) is designed. • Pt/CoP/CNTs exhibit high activity and stability for methanol oxidation reaction(MOR). • The effect of CoP content on electrocatalytic performances for MOR is studied. • CoP decreases the Pt particle size and increases the electrochemical surface areas. • The interaction between Pt and CoP is evidenced by X-ray photoelectron spectroscopy. - Abstract: In this study, carbon nanotubes (CNTs) supported Pt-cobalt phosphide (CoP) electrocatalyst (Pt/CoP/CNTs) is designed and prepared for methanol oxidation (MOR) for the first time. The modification of CoP decreases the Pt particle size significantly and increases the electrochemical surface areas due to the interaction between Pt and CoP, which is evidenced by transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. Among all these catalysts, Pt/4%CoP/CNTs catalyst exhibits the best MOR activity of 1600 mA mg −1 Pt , which is six times that of Pt/CNTs. Moreover, this catalyst also exhibits the higher onset current density and steady current density than the other Pt-based catalysts. The work provides a promising method to develop the highly active and stable Pt-based catalyst for direct methanol fuel cells.

  20. Fabrication of aligned carbon nanotubes on Cu catalyst by dc plasma-enhanced catalytic decomposition

    Energy Technology Data Exchange (ETDEWEB)

    Zhang Zhejuan [Department of Physics, Engineering Research Center for Nanophotonics and Advanced Instrument, East China Normal University, North Zhongshan Road 3663, 200062 Shanghai (China); Shakerzadeh, Maziar; Tay, Beng Kang; Li Xiaocheng; Tan Chongwei [School of Electrical and Electronic Engineering, Nanyang Technological University, Nanyang Avenue 50, 639798 Singapore (Singapore); Lin Lifeng; Guo Pingsheng; Feng Tao [Department of Physics, Engineering Research Center for Nanophotonics and Advanced Instrument, East China Normal University, North Zhongshan Road 3663, 200062 Shanghai (China); Sun Zhuo, E-mail: zsun@phy.ecnu.edu.cn [Department of Physics, Engineering Research Center for Nanophotonics and Advanced Instrument, East China Normal University, North Zhongshan Road 3663, 200062 Shanghai (China)

    2009-04-01

    Aligned multi-walled carbon nanotubes (ACNTs) are deposited using copper (Cu) catalyst on Chromium (Cr)-coated substrate by plasma-enhanced chemical vapor deposition at temperature of 700 deg. C. Acetylene gas has been used as the carbon source while ammonia is used for diluting and etching. The thicknesses of Cu films on Cr-coated Si (100) substrates are controlled by deposition time of magnetron sputtering. The growth behaviors and quality of ACNTs are investigated by scanning electron microscopy (SEM) and transmission electron microscopy. The different performance of ACNTs on various Cu films is explained by referring to the graphitic order as detected by Raman spectroscopy. The results indicate that the ACNTs are formed in tip-growth model where Cu is used as a novel catalyst, and the thickness of Cu films is responsible to the diameter and quality of synthesized CNTs.

  1. Synthesis of vertical MnO{sub 2} wire arrays on hemp-derived carbon for efficient and robust green catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Yang, MinHo [Department of Materials Science and Engineering and Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana–Champaign, Urbana, IL 61801 (United States); Kim, Dong Seok; Sim, Jae-Wook [Department of Chemical Engineering, Kangwon National University, 346 Joongang-ro, Samcheok, Gangwon-do 25913 (Korea, Republic of); Jeong, Jae-Min; Kim, Do Hyun [Department of Chemical & Biomolecular Engineering, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon 34141 (Korea, Republic of); Choi, Jae Hyung [Department of Chemical Engineering, Kangwon National University, 346 Joongang-ro, Samcheok, Gangwon-do 25913 (Korea, Republic of); Department of Chemical Engineering, Pukyong National University, 365 Sinseon-ro, Nam-gu, Busan 48513 (Korea, Republic of); Kim, Jinsoo [Department of Chemical Engineering, Kyung Hee University, 1732, Daogyong-daero, Giheung-gu, Yongin, Gyeonggi-do 17104 (Korea, Republic of); Kim, Seung-Soo, E-mail: sskim2008@kangwon.ac.kr [Department of Chemical Engineering, Kangwon National University, 346 Joongang-ro, Samcheok, Gangwon-do 25913 (Korea, Republic of); Choi, Bong Gill, E-mail: bgchoi@kangwon.ac.kr [Department of Chemical Engineering, Kangwon National University, 346 Joongang-ro, Samcheok, Gangwon-do 25913 (Korea, Republic of)

    2017-06-15

    Highlights: • The three-dimensional nanocomposites based on vertical MnO{sub 2} array on hemp-derived carbon (HDC) were prepared by hydrothermal method. • The 3D v-MnO{sub 2}/HDC nanocomposites showed well-defined porous nature with a high specific surface area of 382.3 m{sup 2} g{sup −1}. • PET glycolysis was performed using the 3D v-MnO{sub 2}/HDC nanocomposites as a catalyst, leading to efficient catalytic performance. - Abstract: Three-dimensional (3D) carbon materials derived from waste biomass have been attracted increasing attention in catalysis and materials science because of their great potential of catalyst supports with respect to multi-functionality, unique structures, high surface area, and low cost. Here, we present a facile and efficient way for preparing 3D heterogeneous catalysts based on vertical MnO{sub 2} wires deposited on hemp-derived 3D porous carbon. The 3D porous carbon materials are fabricated by carbonization and activation processes using hemp (Cannabis Sttiva L.). These 3D porous carbon materials are employed as catalyst supports for direct deposition of vertical MnO{sub 2} wires using a one-step hydrothermal method. The XRD and XPS results reveal the crystalline structure of α-MnO{sub 2} wires. The resultant composites are further employed as a catalyst for glycolysis of poly(ethylene terephthalate) (PET) with high conversion yield of 98%, which is expected to be expressly profitable for plastics recycling industry.

  2. 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

    2016-02-08

    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. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. 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...... membrane fuel cell based on H3PO4-doped PBI for operation at temperatures between 150 and 200 degrees C. (C) 2000 Elsevier Science Ltd. All rights reserved....

  4. 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....

  5. 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.

  6. Revealing the Dynamics of Platinum Nanoparticle Catalysts on Carbon in Oxygen and Water Using Environmental TEM

    Energy Technology Data Exchange (ETDEWEB)

    Luo, Langli [Environmental; Engelhard, Mark H. [Environmental; Shao, Yuyan [Environmental; Wang, Chongmin [Environmental

    2017-10-02

    Deactivation of supported metal nanoparticle catalysts, especially in relevant gas condition, is a critical challenge for many technological applications, including heterogeneous catalysis, electrocatalysis, fuel cells, biomedical imaging and drug delivery. It has been far more commonly realized that deactivation of catalysts stems from surface area loss due to particle coarsening, however, for which the mechanism remains largely unclear. Herein, we use aberration corrected environmental transmission electron microscopy, at atomic level, to in-situ observe the dynamics of Pt catalyst in fuel cell relevant gas conditions. Particles migration and coalescence is observed to be the dominant coarsening process. As compared with the case of H2O, O2 promotes Pt nanoparticle migration on carbon surface. Surprisingly, coating Pt/carbon with a nanofilm of electrolyte (Nafion ionomer) leads to a faster migration of Pt in H2O than in O2, a consequence of Nafion-carbon interface water “lubrication” effect. Atomically, the particles coalescence is featured by re-orientation of particles towards lattice matching, a process driven by orientation dependent van der Waals force. These results provide direct observations of dynamics of metal nanoparticles at critical surface/interface under relevant conditions and yield significant insights into the multi-phase interaction in related technological processes.

  7. A facile approach towards increasing the nitrogen-content in nitrogen-doped carbon nanotubes via halogenated catalysts

    International Nuclear Information System (INIS)

    Ombaka, L.M.; Ndungu, P.G.; Omondi, B.; McGettrick, J.D.; Davies, M.L.; Nyamori, V.O.

    2016-01-01

    Nitrogen-doped carbon nanotubes (N-CNTs) have been synthesized at 850 °C via a CVD deposition technique by use of three ferrocenyl derivative catalysts, i.e. para-CN, -CF_3 and -Cl substituted-phenyl rings. The synthesized catalysts have been characterized by NMR, IR, HR-MS and XRD. The XRD analysis of the para-CF_3 catalyst indicates that steric factors influence the X-ray structure of 1,1′-ferrocenylphenyldiacrylonitriles. Acetonitrile or pyridine was used as carbon and nitrogen sources to yield mixtures of N-CNTs and carbon spheres (CS). The N-CNTs obtained from the para-CF_3 catalysts, in pyridine, have the highest nitrogen-doping level, show a helical morphology and are less thermally stable compared with those synthesized by use of the para-CN and -Cl as catalyst. This suggests that fluorine heteroatoms enhance nitrogen-doping in N-CNTs and formation of helical-N-CNTs (H-N-CNTs). The para-CF_3 and para-Cl catalysts in acetonitrile yielded iron-filled N-CNTs, indicating that halogens promote encapsulation of iron into the cavity of N-CNT. The use of acetonitrile, as carbon and nitrogen source, with the para-CN and -Cl as catalysts also yielded a mixture of N-CNTs and carbon nanofibres (CNFs), with less abundance of CNFs in the products obtained using para-Cl catalysts. However, para-CF_3 catalyst in acetonitrile gave N-CNTs as the only shaped carbon nanomaterials. - Graphical abstract: Graphical abstract showing the synthesis of N-CNTs using halogenated-ferrocenyl derivatives as catalyst with pyridine or acetonitrile as nitrogen and carbon sources via the chemical vapour deposition technique. - Highlights: • N-CNTs were synthesized from halogenated ferrocenyl catalysts. • Halogenated catalysts promote nitrogen-doping and pyridinic nitrogen in N-CNTs. • Halogenated catalysts facilitate iron filling of N-CNTs.

  8. Study of the effect of different mixed supports on the catalytic activity and the structure of Bi2MoxW1-xO6 catalysts

    International Nuclear Information System (INIS)

    Rangel, R.; Cervantes L, J. L.; Espino, J.; Nunez G, R.; Bartolo P, P.; Gomez C, A.; Diaz, G.

    2014-01-01

    A series of Bi 2 Mo x W 1-x O 6 catalysts supported on Al 2 O 3 -SiO 2 , SiO 2 -TiO 2 and activated carbon were synthesized. The aim was to compare the different supports and calcination temperature of catalysts, studying their efficiency and activation temperature in the CO oxidation reaction. The catalysts active phase, Bi 2 Mo x W 1-x O 6 was made by means of chemical precipitation procedure starting from high purity (NH 4 ) 6 Mo 7 O 24 ·4H 2 O, (NH 4 ) 6 W 12 O 6 ·H 2 O, Bi(NO 3 ) 2 ·5H 2 O compounds, which afterwards, were supported on Al 2 O 3 -SiO 2 , SiO 2 -TiO 2 and activated carbon through impregnation. The catalysts characterization was carried out by means of X-ray diffraction analysis, scanning electron microscopy and surface area determination (Bet method). Regarding the catalytic activity the Bi 2 Mo x W 1-x O 6 /carbon activated compound synthesized at 500 grades C was the best catalyst being activated at 125 grades C reaching 90% conversion. It is concludes that was observed an effect of calcination temperature and the support on the different values reached for the catalytic activity. (Author)

  9. Syntheses of carbon porous materials with varied pore sizes and their performances as catalyst supports during methanol oxidation reaction

    International Nuclear Information System (INIS)

    Lo, An-Ya; Hung, Chin-Te; Yu, Ningya; Kuo, Cheng-Tzu; Liu, Shang-Bin

    2012-01-01

    Highlights: ► CPMs with varied pore sizes (1–400 nm) were replicated from various porous silicas by CVI method. ► MOR activities of Pt/CPM electrocatalysts increase with increasing pore size of CPM support. ► Microporous CPMs are favorable supports for Pt in terms of catalytic performance and CO-tolerance. -- Abstract: Carbon porous materials (CPMs) with extended ranges of pore size and morphology were replicated using various porous silicas, such as zeolites, mesoporous silicas, and photonic crystals, as templates by means of chemical vapor infiltration (CVI) method. The micro-, meso-, and macro-porous carbons so fabricated were adopted as supports for the metal (Pt) catalyst for direct methanol fuel cells (DMFCs), and the supported Pt/CPM electrocatalysts were characterized by a variety of different spectroscopic/analytical techniques, viz. transmission electron microscopy (TEM), Raman, X-ray photoelectron spectroscopy (XPS), gas physisorption/chemisorption analyses, and cyclic voltammetry (CV). That these Pt/CPMs were found to exhibit superior electrocatalytic activities compared to the commercial Pt/XC-72 with a comparable Pt loading during methanol oxidation reaction (MOR) is attributed to the presence of Pt nanoparticles (NPs; typically 1–3 nm in size) that are highly dispersed in the CPMs, facilitating an improved tolerance for CO poisoning. While the MOR activity observed for various Pt/CPMs tend to increase with increasing pore size of the carbon supports, Pt catalyst supported on carbon substrates possessing microporosities was found to have superior stability in terms of tolerance for CO poisoning than those with greater pore size or having meso- and macroporosities.

  10. Partial oxidation of municipal sludge with activited carbon catalyst in supercritical water

    International Nuclear Information System (INIS)

    Guo Yang; Wang Shuzhong; Gong Yanmeng; Xu Donghai; Tang Xingying; Ma Honghe

    2010-01-01

    The partial oxidation (POX) characteristics of municipal sludge in supercritical water (SCW) were investigated by using batch reactor. Effects of reaction parameters such as oxidant equivalent ratio (OER), reaction time and temperature were investigated. Activated carbon (AC) could effectively improve the mole fraction of H 2 in gas product at low OER. However, high OER (greater than 0.3) not only led to the combustion reaction of CO and H 2 , but also caused corrosion of reactor inner wall. Hydrogenation and polymerization of the intermediate products are possible reasons for the relative low COD removal rate in our tests. Metal oxide leached from the reactor inner wall and the main components of the granular sludge were deposited in the AC catalyst. Reaction time had more significant effect on BET surface area of AC than OER had. Long reaction time led to the methanation reaction following hydrolysis and oxidation reaction of AC in SCW in the presence of oxygen. Correspondingly, the possible reaction mechanisms were proposed.

  11. Multifunctional Interlayer Based on Molybdenum Diphosphide Catalyst and Carbon Nanotube Film for Lithium-Sulfur Batteries.

    Science.gov (United States)

    Luo, Yufeng; Luo, Nannan; Kong, Weibang; Wu, Hengcai; Wang, Ke; Fan, Shoushan; Duan, Wenhui; Wang, Jiaping

    2018-02-01

    A multifunctional interlayer, composed of molybdenum diphosphide (MoP 2 ) nanoparticles and a carbon nanotube (CNT) film, is introduced into a lithium-sulfur (Li-S) battery system to suppress polysulfide migration. Molybdenum diphosphide acts as the catalyst and can capture polysulfides and improve the polysulfide conversion activity during the discharge/charge processes. The CNT film acts as a conductive skeleton to support the MoP 2 nanoparticles and to ensure their uniform distribution. The CNT film physically hinders polysulfide migration, acts as a current collector, and provides abundant electron pathways. The Li-S battery containing the multifunctional MoP 2 /CNT interlayer exhibits excellent electrochemical performance. It delivers a reversible specific capacity of 905 mA h g -1 over 100 cycles at 0.2 C, with a capacity decay of 0.152% per cycle. These results suggest the introduction of the multifunctional CNT/MoP 2 interlayer as an effective and practical method for producing high-performance Li-S batteries. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Catalysts for synthetic liquid fuels

    Energy Technology Data Exchange (ETDEWEB)

    Bruce, L.A.; Turney, T.W.

    1987-12-01

    Fischer-Tropsch catalysts have been designed, characterized and tested for the selective production of hydrocarbons suitable as synthetic liquid transport fuels from synthesis gas (i.e., by the reduction of carbon monoxide with hydrogen). It was found that hydrocarbons in the middle distillate range, or suitable for conversion to that range, could be produced over several of the new catalyst systems. The various catalysts examined included: (1) synthetic cobalt clays, mainly cobalt chlorites; (2) cobalt hydrotalcites; (3) ruthenium metal supported on rare earth oxides of high surface area; and (4) a novel promoted cobalt catalyst. Active and selective catalysts have been obtained, in each category. With the exception of the clays, reproducibility of catalyst performance has been good. Catalysts in groups 2 and 4 have exhibited very high activity, with long lifetimes and easy regeneration.

  13. 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.

  14. Metal-Doped Nitrogenated Carbon as an Efficient Catalyst for Direct CO2 Electroreduction to CO and Hydrocarbons.

    Science.gov (United States)

    Varela, Ana Sofia; Ranjbar Sahraie, Nastaran; Steinberg, Julian; Ju, Wen; Oh, Hyung-Suk; Strasser, Peter

    2015-09-07

    This study explores the kinetics, mechanism, and active sites of the CO2 electroreduction reaction (CO2RR) to syngas and hydrocarbons on a class of functionalized solid carbon-based catalysts. Commercial carbon blacks were functionalized with nitrogen and Fe and/or Mn ions using pyrolysis and acid leaching. The resulting solid powder catalysts were found to be active and highly CO selective electrocatalysts in the electroreduction of CO2 to CO/H2 mixtures outperforming a low-area polycrystalline gold benchmark. Unspecific with respect to the nature of the metal, CO production is believed to occur on nitrogen functionalities in competition with hydrogen evolution. Evidence is provided that sufficiently strong interaction between CO and the metal enables the protonation of CO and the formation of hydrocarbons. Our results highlight a promising new class of low-cost, abundant electrocatalysts for synthetic fuel production from CO2 . © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  15. A phenyl-sulfonic acid anchored carbon-supported platinum catalyst for polymer electrolyte fuel cell electrodes

    International Nuclear Information System (INIS)

    Selvarani, G.; Sahu, A.K.; Choudhury, N.A.; Sridhar, P.; Pitchumani, S.; Shukla, A.K.

    2007-01-01

    A method, to anchor phenyl-sulfonic acid functional groups with the platinum catalyst supported onto a high surface-area carbon substrate, is reported. The use of the catalyst in the electrodes of a polymer electrolyte fuel cell (PEFC) helps enhancing its performance. Characterization of the catalyst by Fourier transform infra red (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS) and point-of-zero-charge (PZC) studies suggests that the improvement in performance of the PEFC is facilitated not only by enlarging the three-phase boundary in the catalyst layer but also by providing ionic-conduction paths as well as by imparting negative charge to platinum sites with concomitant oxidation of sulfur present in the carbon support. It is argued that the negatively charged platinum sites help repel water facilitating oxygen to access the catalyst sites. The PEFC with modified carbon-supported platinum catalyst electrodes exhibits 40% enhancement in its power density as compared to the one with unmodified carbon-supported platinum catalyst electrodes

  16. Graphene Carbon Nanotube Carpets Grown Using Binary Catalysts for High-Performance Lithium-Ion Capacitors.

    Science.gov (United States)

    Salvatierra, Rodrigo Villegas; Zakhidov, Dante; Sha, Junwei; Kim, Nam Dong; Lee, Seoung-Ki; Raji, Abdul-Rahman O; Zhao, Naiqin; Tour, James M

    2017-03-28

    Here we show that a versatile binary catalyst solution of Fe 3 O 4 /AlO x nanoparticles enables homogeneous growth of single to few-walled carbon nanotube (CNT) carpets from three-dimensional carbon-based substrates, moving past existing two-dimensional limited growth methods. The binary catalyst is composed of amorphous AlO x nanoclusters over Fe 3 O 4 crystalline nanoparticles, facilitating the creation of seamless junctions between the CNTs and the underlying carbon platform. The resulting graphene-CNT (GCNT) structure is a high-density CNT carpet ohmically connected to the carbon substrate, an important feature for advanced carbon electronics. As a demonstration of the utility of this approach, we use GCNTs as anodes and cathodes in binder-free lithium-ion capacitors, producing stable devices with high-energy densities (∼120 Wh kg -1 ), high-power density capabilities (∼20,500 W kg -1 at 29 Wh kg -1 ), and a large operating voltage window (4.3 to 0.01 V).

  17. Synthesis of biodiesel from waste vegetable oil with large amounts of free fatty acids using a carbon-based solid acid catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Shu, Qing; Gao, Jixian; Nawaz, Zeeshan; Liao, Yuhui; Wang, Dezheng; Wang, Jinfu [Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084 (China)

    2010-08-15

    A carbon-based solid acid catalyst was prepared by the sulfonation of carbonized vegetable oil asphalt. This catalyst was employed to simultaneously catalyze esterification and transesterification to synthesis biodiesel when a waste vegetable oil with large amounts of free fatty acids (FFAs) was used as feedstock. The physical and chemical properties of this catalyst were characterized by a variety of techniques. The maximum conversion of triglyceride and FFA reached 80.5 wt.% and 94.8 wt.% after 4.5 h at 220 C, when using a 16.8 M ratio of methanol to oil and 0.2 wt.% of catalyst to oil. The high catalytic activity and stability of this catalyst was related to its high acid site density (-OH, Broensted acid sites), hydrophobicity that prevented the hydration of -OH species, hydrophilic functional groups (-SO{sub 3}H) that gave improved accessibility of methanol to the triglyceride and FFAs, and large pores that provided more acid sites for the reactants. (author)

  18. Contribution to the study of the oxidation reaction of the carbon oxide in contact with catalysts issued from the decomposition of nickel hydro-aluminates at various temperatures

    International Nuclear Information System (INIS)

    Samaane, Mikhail

    1966-01-01

    Addressing the study of the oxidation reaction of carbon oxide which produces carbon dioxide, this research thesis reports the study of this reaction in presence of catalysts (2NiO + Al 2 O 3 , NiAl 2 O 4 and NiO + NiAl 2 O 4 ) issued from the decomposition of nickel hydro-aluminates at different temperatures. The first part describes experimental techniques and the nature of materials used in this study. The second part reports the study of the catalytic activity of the 2NiO+Al 2 O 3 catalyst during the oxidation of CO. Preliminary studies are also reported: structure and texture of nickel hydro-aluminate which is the raw material used to produce catalysts, activation of this compound to develop the catalytic activity in CO oxidation, chemisorption of CO, O 2 and CO 2 on the 2NiO+Al 2 O 3 solid, interaction of adsorbed gases at the solid surface, and kinetic study of the oxidation reaction. The third part reports the study of the catalytic activity in the oxidation reaction of CO of spinel catalysts (NiAl 2 O 4 and NiO+NiAl 2 O 4 ) obtained by calcination of nickel hydro-aluminates at high temperature. The formation of the spinel phase, the chemisorption of CO, O 2 and CO 2 on NiAl 2 O 4 , and the kinetic of the oxidation reaction are herein studied

  19. Catalytic activity of mono and bimetallic Zn/Cu/MWCNTs catalysts for the thermocatalyzed conversion of methane to hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Erdelyi, B. [Department of Physical Chemistry, Faculty of Science, P.J. Šafárik University, Moyzesova 11, 041 54 Košice (Slovakia); Institute of Physics, Faculty of Science, P.J. Šafárik University, Park Angelium 9, 040 01 Košice (Slovakia); Oriňak, A., E-mail: andrej.orinak@upjs.sk [Department of Physical Chemistry, Faculty of Science, P.J. Šafárik University, Moyzesova 11, 041 54 Košice (Slovakia); Oriňaková, R. [Department of Physical Chemistry, Faculty of Science, P.J. Šafárik University, Moyzesova 11, 041 54 Košice (Slovakia); Lorinčík, J. [Research Center Rez, Hlavní 130, 250 68 Husinec-Řež (Czech Republic); Jerigová, M. [Department of Physical Chemistry, Comenius University, Mlynská dolina 842 15 Bratislava 4 (Slovakia); Velič, D. [Department of Physical Chemistry, Comenius University, Mlynská dolina 842 15 Bratislava 4 (Slovakia); International Laser Centre, Ilkovičová 3, 841 01 Bratislava (Slovakia); Mičušík, M. [Polymer institute, Slovak Academy of Sciences, Dubravská cesta 9, 84541 Bratislava (Slovakia); and others

    2017-02-28

    Highlights: • Zn/Cu/MWCNTs catalyst with good activity. • Methane conversion to hydrogen with high effectivity. • ZnO/Cu responsible for catalytic activity. - Abstract: Mono and bimetallic multiwalled carbon nanotubes (MWCNTs) fortified with Cu and Zn metal particles were studied to improve the efficiency of the thermocatalytic conversion of methane to hydrogen. The surface of the catalyst and the dispersion of the metal particles were studied by scanning electron microscopy (SEM), secondary ion mass spectrometry (SIMS) and with energy-dispersive X-ray spectroscopy (EDS). It was confirmed that the metal particles were successfully dispersed on the MWCNT surface and XPS analysis showed that the Zn was oxidised to ZnO at high temperatures. The conversion of methane to hydrogen during the catalytic pyrolysis was studied by pyrolysis gas chromatography using different amounts of catalyst. The best yields of hydrogen were obtained using pyrolysis conditions of 900 °C and 1.2 mg of Zn/Cu/MWCNT catalyst for 1.5 mL of methane.The initial conversion of methane to hydrogen obtained with Zn/Cu/MWCNTs was 49%, which represent a good conversion rate of methane to hydrogen for a non-noble metal catalyst.

  20. Carbon Nitride Materials as Efficient Catalyst Supports for Proton Exchange Membrane Water Electrolyzers

    Directory of Open Access Journals (Sweden)

    Ana Belen Jorge

    2018-06-01

    Full Text Available Carbon nitride materials with graphitic to polymeric structures (gCNH were investigated as catalyst supports for the proton exchange membrane (PEM water electrolyzers using IrO2 nanoparticles as oxygen evolution electrocatalyst. Here, the performance of IrO2 nanoparticles formed and deposited in situ onto carbon nitride support for PEM water electrolysis was explored based on previous preliminary studies conducted in related systems. The results revealed that this preparation route catalyzed the decomposition of the carbon nitride to form a material with much lower N content. This resulted in a significant enhancement of the performance of the gCNH-IrO2 (or N-doped C-IrO2 electrocatalyst that was likely attributed to higher electrical conductivity of the N-doped carbon support.

  1. Composite supercapacitor electrodes made of activated carbon ...

    Indian Academy of Sciences (India)

    carbon/PEDOT:PSS and activated carbon/doped PEDOT. T S SONIA, P A MINI, ... polymeric anodes for organic photovoltaics, light-emitting diodes (Pingree et al ... looked upon are carbon nanotubes (CNTs), graphene and activated carbon.

  2. Preparation and Characterization of Pd Modified TiO2 Nanofiber Catalyst for Carbon–Carbon Coupling Heck Reaction

    Directory of Open Access Journals (Sweden)

    Leah O. Nyangasi

    2017-01-01

    Full Text Available TiO2 fibers were prepared through electrospinning of poly methyl methacrylate (PMMA and titanium isopropoxide (TIP solution followed by calcination of fibers in air at 500°C. Cetyltrimethylammonium bromide (CTAB protected palladium nanoparticles (Pd NPs prepared through reduction method were successfully adsorbed on the TiO2 nanofibers (NF. Combined studies of X-ray diffraction (XRD, scanning electron microscope (SEM, and transmission electron microscope (TEM indicated that the synthesized Pd/TiO2 had anatase. BET indicated that the synthesized TiO2 and Pd/TiO2 had a surface area of 53.4 and 43.4 m2/g, respectively. The activity and selectivity of 1 mol% Pd/TiO2 in the Heck reaction have been investigated towards the Mizoroki-Heck carbon–carbon cross-coupling of bromobenzene (ArBr and styrene. Temperature, time, solvent, and base were optimized and catalyst was recycled thrice. 1H NMR and 13C NMR indicated that stilbene, a known compound from literature, was obtained in various Heck reactions at temperatures between 100°C and 140°C but the recyclability was limited due to some palladium leaching and catalyst poisoning which probably arose from some residual carbon from the polymer. The catalyst was found to be highly active under air atmosphere with reaction temperatures up to 140°C. Optimized reaction condition resulted in 89.7% conversions with a TON of 1993.4 and TOF value of 332.2 hr−1.

  3. Niobium(v) chloride and imidazolium bromides as efficient dual catalyst systems for the cycloaddition of carbon dioxide and propylene oxide

    KAUST Repository

    Wilhelm, Michael E.; Anthofer, Michael H.; Reich, Robert M.; D'Elia, Valerio; Basset, Jean-Marie; Herrmann, Wolfgang A.; Cokoja, Mirza; Kü hn, Fritz

    2014-01-01

    The application of niobium(v) chloride and several imidazolium bromides as catalyst systems for the cycloaddition of propylene oxide (PO) with carbon dioxide to propylene carbonate (PC) is reported. A set of 31 different imidazolium bromides has been synthesized with varying substituents at all five imidazolium ring atoms, of which 17 have not been reported before. The impact of different substitution patterns (steric and electronic changes and solubility in PO) at the imidazolium ring on the catalytic activity was investigated. The optimisation of the catalyst structure allows for the valorisation of carbon dioxide under mild reaction conditions with high reaction rates in very good yield and selectivity for PC. This journal is © the Partner Organisations 2014.

  4. Niobium(v) chloride and imidazolium bromides as efficient dual catalyst systems for the cycloaddition of carbon dioxide and propylene oxide

    KAUST Repository

    Wilhelm, Michael E.

    2014-02-19

    The application of niobium(v) chloride and several imidazolium bromides as catalyst systems for the cycloaddition of propylene oxide (PO) with carbon dioxide to propylene carbonate (PC) is reported. A set of 31 different imidazolium bromides has been synthesized with varying substituents at all five imidazolium ring atoms, of which 17 have not been reported before. The impact of different substitution patterns (steric and electronic changes and solubility in PO) at the imidazolium ring on the catalytic activity was investigated. The optimisation of the catalyst structure allows for the valorisation of carbon dioxide under mild reaction conditions with high reaction rates in very good yield and selectivity for PC. This journal is © the Partner Organisations 2014.

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

    KAUST Repository

    Xu, Xuezhu; Zhou, Jian; Nagaraju, Doddahalli H.; Jiang, Long; Marinov, Val R.; Lubineau, Gilles; Alshareef, Husam N.; Oh, Myungkeun

    2015-01-01

    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

  6. Single Pot Selective Hydrogenation of Furfural to 2-Methylfuran Over Carbon Supported Iridium Catalysts

    KAUST Repository

    Date, Nandan S; Hengne, Amol Mahalingappa; Huang, Kuo-Wei; Chikate, Rajeev C.; Rode, C. V.

    2018-01-01

    Various iridium supported carbon catalysts were prepared and screened for direct hydrogenation of furfural (FFR) to 2-methyl furan (2-MF). Amongest these, 5% Ir/C showed excellent results with complete FFR conversion and highest selectivity of 95% to 2-MF at very low H2 pressure of 100 psig. Metallic (Iro) and oxide ( IrO2) phases of Ir catalyzed first step hydrogenation involving FFR to FAL and subsequent hydrogenation to 2-MF,respecively. This was confirmed by XPS analysis and some controlled experiments. At low temperature of 140 oC, almost equal selectivities of FAL (42%) and 2-MF (43%) were observed, while higher temperature (220oC) favored selective hydrodeoxygenation. At optimized temperature, 2-MF formed selectively while higher pressure and higher catalyst loading favored ring hydrogenation of furfural rather than side chain hydrogenation. With combination of several control experimental results and detailed catalyst characterization, a plausible reaction pathway has been proposed for selective formation of 2-MF. The selectivity to various other products in FFR hydrogenation can be manipulated by tailoring the reaction conditions over the same catalyst.

  7. Surface heterogeneity and ionization of Cs promoter in carbon-based ruthenium catalyst for ammonia synthesis

    International Nuclear Information System (INIS)

    Kotarba, Andrzej; Dmytrzyk, Jaromir; Rarog-Pilecka, Wioletta; Kowalczyk, Zbigniew

    2003-01-01

    Second-generation ammonia synthesis cesium-doped ruthenium catalyst supported on turbostratic carbon was investigated by the species resolved thermal alkali desorption method (SR-TAD). Energetic barriers for cesium ions (2.86 eV), ground state (1.96 eV) and electronically excited atoms (5.76 eV) desorbing from the Cs-Ru/C catalyst were determined. In the case of ruthenium-free Cs/C system, cesium desorbs as ground state atoms only, with an energy barrier of 2.87 eV. The work functions determined by the thermionic emission of electrons from Cs/C and Cs-Ru/C were of the same value (2.9 eV). It was concluded that ruthenium induces heterogeneous distribution of cesium on the catalyst surface. The promoter stability is reduced on low work function areas and its surface ionization on high work function areas opens the ionic desorption channel. The Cs desorption from the catalyst is discussed in terms of the literature data for the cesium/graphite system

  8. Single Pot Selective Hydrogenation of Furfural to 2-Methylfuran Over Carbon Supported Iridium Catalysts