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)

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.

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.

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.

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.

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.

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...

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.

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.

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.

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.

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

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

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

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.

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.

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)

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.

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)

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)

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.

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.

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.

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.

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.

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)

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...

De-oxygenation of CO2 by using Hydrogen, Carbon and Methane over Alumina-Supported Catalysts

Directory of Open Access Journals (Sweden)

R.Y. Raskar

2012-06-01

Full Text Available The de-oxygenation of CO2 was explored by using hydrogen, methane, carbon etc., over alumina supported catalysts. The alumina-supported ruthenium, rhodium, platinum, molybdenum, vanadium and magnesium catalysts were first reduced in hydrogen atmosphere and then used for the de-oxygenation of CO2. Furthermore, experimental variables for the de-oxygenation of CO2 were temperature (range 50 to 650 oC, H2/CO2 mole ratios (1.0 to 5, and catalyst loading (0.5 to 10 wt %. During the de-oxygenation of CO2 with H2 or CH4 or carbon, conversion of CO2, selectivity to CO and CH4 were estimated. Moreover, 25.4 % conversion of CO2 by hydrogen was observed over 1 wt% Pt/Al2O3 catalyst at 650 oC with 33.8 % selectivity to CH4. However, 8.1 to 13.9 % conversion of CO2 was observed over 1 wt% Pt/Al2O3 catalyst at 550 oC in the presence of both H2 and CH4. Moreover, 42.8 to 79.4 % CH4 was converted with 9 to 23.1 % selectivity to CO. It was observed that the de-oxygenation of CO2 by hydrogen, carbon and methane produced carbon, CO and CH4. © 2012 BCREC UNDIP. All rights reservedReceived: 6th February 2012; Revised: 23rd April 2012; Accepted: 24th April 2012[How to Cite: R. Y. Raskar, K. B. Kale, A. G. Gaikwad. (2011. De-oxygenation of CO2 by using Hydrogen, Carbon and Methane over Alumina-Supported Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 7 (1: 59-69.  doi:10.9767/bcrec.7.1.1631.59-69][How to Link / DOI: http://dx.doi.org/10.9767/bcrec.7.1.1631.59-69 ] | View in 

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.

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...

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.

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.

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)

Thermal and electrochemical stability of tungsten carbide catalyst supports

Energy Technology Data Exchange (ETDEWEB)

Chhina, H. [Ballard Power Systems, 9000 Glenlyon Parkway, Burnaby, BC (Canada); Department of Materials Engineering, University of British Columbia, Vancouver, BC (Canada); Campbell, S. [Ballard Power Systems, 9000 Glenlyon Parkway, Burnaby, BC (Canada); Kesler, O. [Department of Mechanical Engineering, University of British Columbia, Vancouver, BC (Canada)

2007-02-10

The thermal and electrochemical stability of tungsten carbide (WC), with and without a catalyst dispersed on it, have been investigated to evaluate the potential suitability of the material as an oxidation-resistant catalyst support. Standard techniques currently used to disperse Pt on carbon could not be used to disperse Pt on WC, so an alternative method was developed and used to disperse Pt on both commercially available WC and on carbon for comparison of stability. Electrochemical testing was performed by applying oxidation cycles between +0.6 V and +1.8 V to the support-catalyst material combinations and monitoring the activity of the supported catalyst over 100 oxidation cycles. Comparisons of activity change with cumulative oxidation cycles were made between C and WC supports with comparable loadings of catalyst by weight, solid volume, and powder volume. WC was found to be more thermally and electrochemically stable than currently used carbon support material Vulcan XC-72R. However, further optimization of the particle sizes and dispersion of Pt/WC catalyst/support materials and of comparison standards between new candidate materials and existing carbon-based supports are required. (author)

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)

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)

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

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

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.

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...

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.

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.

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.

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.

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...

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.

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.

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.

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.

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...

The effect of promoters on the electronic structure of ruthenium catalysts supported on carbon

International Nuclear Information System (INIS)

Guraya, Monica; Sprenger, Susanne; Rarog-Pilecka, Wioletta; Szmigiel, Dariusz; Kowalczyk, Zbigniew; Muhler, Martin

2004-01-01

Alkali- and earth-alkali-promoted ruthenium catalysts supported on graphitized carbon were investigated by means of X-ray and ultraviolet photoelectron spectroscopy (XPS and UPS) in order to study the effect of promoters on the electronic structure of this metal-support system. Samples were measured as prepared and after thorough reduction in hydrogen. The C 1s spectra of reduced alkali-promoted catalysts showed a shift towards higher binding energies and an asymmetric broadening. Neither non-promoted nor Ba-promoted Ru/C samples exhibited such a behaviour after similar treatments. The most important feature in the UP spectra of the reduced alkali-promoted catalysts was the appearance of a well defined Fermi edge absent in the semimetal-like electronic structure of graphite. No significant effects appeared in the case of non-promoted or Ba-promoted catalysts. The increase in the density of occupied states at the Fermi energy indicates a shift of this level into the conduction band, due to a charge transfer from the promoter to the support. This interpretation also provides an explanation for the observed higher C 1s binding energy and asymmetric broadening, due to the off-set introduced in the binding energy scale and the increasing probability of inelastic excitations near the Fermi level. In addition to photoelectron spectroscopy, low energy ion scattering (ISS) was used to obtain information about the localisation of the promoters. Based on the mild sputtering effect during prolonged series of spectra, it was possible to conclude that potassium covers both the carbon support and the Ru metal particles

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

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.

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

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)

Synthesis of honeycomb-like mesoporous nitrogen-doped carbon nanospheres as Pt catalyst supports for methanol oxidation in alkaline media

Science.gov (United States)

Zhang, Yunmao; Liu, Yong; Liu, Weihua; Li, Xiying; Mao, Liqun

2017-06-01

This paper reports the convenient synthesis of honeycomb-like mesoporous nitrogen-doped carbon spheres (MNCS) using a self-assembly strategy that employs dopamine (DA) as a carbon and nitrogen precursor and a polystyrene-b-poly(ethylene oxide) (PS173-b-PEO170) diblock copolymer as a soft template. The MNCS have large BET surface areas of up to 554 m2 g-1 and high nitrogen contents of up to 6.9 wt%. The obtained MNCS are used as a support for Pt catalysts, which promote methanol oxidation in alkaline media. The MNCS-supported Pt (Pt/MNCS) catalyst has a larger electrochemically active surface area (ESA) (89.2 m2 g-1) than does a commercially available Vulcan XC-72R supported Pt/C catalyst. Compared to the Pt/C catalyst, Pt/MNCS displays a higher peak current density (1007 mA mg-1) and is more stable during methanol oxidation. These improvements are attributed to the honeycomb-like porous structure of the MNCS and the introduction of nitrogen to the carbon support. The MNCS effectively stabilize Pt nanoparticles and assuage the agglomeration of the nanoparticles, suggesting that MNCS are potential and promising application as electrocatalyst supports in alkaline direct methanol fuel cells.

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

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.

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.

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.)

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.

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...

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....

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.

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.

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.

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.

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.

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...

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.

Comparison study of catalyst nanoparticle formation and carbon nanotube growth: Support effect

International Nuclear Information System (INIS)

Wang Yunyu; Luo Zhiquan; Li Bin; Ho, Paul S.; Yao Zhen; Shi Li; Bryan, Eugene N.; Nemanich, Robert J.

2007-01-01

A comparison study has been conducted on the formation of catalyst nanoparticles on a high surface tension metal and low surface tension oxide for carbon nanotube (CNT) growth via catalytic chemical vapor deposition (CCVD). Silicon dioxide (SiO 2 ) and tantalum have been deposited as supporting layers before deposition of a thin layer of iron catalyst. Iron nanoparticles were formed after thermal annealing. It was found that densities, size distributions, and morphologies of iron nanoparticles were distinctly different on the two supporting layers. In particular, iron nanoparticles revealed a Volmer-Weber growth mode on SiO 2 and a Stranski-Krastanov mode on tantalum. CCVD growth of CNTs was conducted on iron/tantalum and iron/SiO 2 . CNT growth on SiO 2 exhibited a tip growth mode with a slow growth rate of less than 100 nm/min. In contrast, the growth on tantalum followed a base growth mode with a fast growth rate exceeding 1 μm/min. For comparison, plasma enhanced CVD was also employed for CNT growth on SiO 2 and showed a base growth mode with a growth rate greater than 2 μm/min. The enhanced CNT growth rate on tantalum was attributed to the morphologies of iron nanoparticles in combination with the presence of an iron wetting layer. The CNT growth mode was affected by the adhesion between the catalyst and support as well as CVD process

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....

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.

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.

Surface tailored single walled carbon nanotubes as catalyst support for direct methanol fuel cell

Science.gov (United States)

Kireeti, Kota V. M. K.; Jha, Neetu

2017-10-01

A strategy for tuning the surface property of Single Walled Carbon Nanotubes (SWNTs) for enhanced methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR) along with methanol tolerance is presented. The surface functionality is tailored using controlled acid and base treatment. Acid treatment leads to the attachment of carboxylic carbon (CC) fragments to SWNT making it hydrophilic (P3-SWNT). Base treatment of P3-SWNT with 0.05 M NaOH reduces the CCs and makes it hydrophobic (P33-SWNT). Pt catalyst supported on the P3-SWNT possesses enhanced MOR whereas that supported on P33-SWNT not only enhances ORR kinetics but also possess good tolerance towards methanol oxidation as verified by the electrochemical technique.

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.

Iron-57 and iridium-193 Moessbauer spectroscopic studies of supported iron-iridium catalysts

International Nuclear Information System (INIS)

Berry, F.J.; Jobson, S.

1988-01-01

57 Fe and 193 Ir Moessbauer spectroscopy shows that silica- and alumina-supported iron-iridium catalysts formed by calcination in air contain mixtures of small particle iron(III) oxide and iridium(IV) oxide. The iridium dioxide in both supported catalysts is reduced in hydrogen to metallic iridium. The α-Fe 2 O 3 in the silica supported materials is predominantly reduced in hydrogen to an iron-iridium alloy whilst in the alumina-supported catalyst the iron is stabilised by treatment in hydrogen as iron(II). Treatment of a hydrogen-reduced silica-supported iron catalyst in hydrogen and carbon monoxide is accompanied by the formation of iron carbides. Carbide formation is not observed when the iron-iridium catalysts are treated in similar atmospheres. The results from the bimetallic catalysts are discussed in terms of the hydrogenation of associatively adsorbed carbon monoxide and the selectivity of supported iron-iridium catalysts to methanol formation. (orig.)

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.

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.

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...

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.

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.

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.

Single Pot Selective Hydrogenation of Furfural to 2-Methylfuran Over Carbon Supported Iridium Catalysts

KAUST Repository

Date, Nandan S

2018-03-20

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.

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)

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.

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

Wire gauze and cordierite supported noble metal catalysts for passive autocatalytic recombiner

International Nuclear Information System (INIS)

Sanap, Kiran K.; Varma, S.; Waghmode, S.B.; Bharadwaj, S.R.

2015-01-01

Highlights: • Synthesis by electroless deposition method and chemical reduction route. • Particle size of 0.1–0.5 μm & 3.5–5 nm for Pt–Pd/Wg & Pt–Pd/Cord catalysts. • Active for H_2 and O_2 reaction with initial H_2 concentration of 1.5 to 7% in air. • Active in presence of different contaminants like CO_2, CH_4, CO & relative humidity. • Enhanced resistance of Pt–Pd/Cord catalyst towards the poisoning of CO. - Abstract: Hydrogen released in nuclear reactor containment under severe accident scenario poses a threat to containment and hence needs to be regulated by catalytic recombination. Mixed noble metal catalysts with platinum–palladium supported on stainless steel wire gauze and cordierite support have been developed for this purpose. The developed catalysts have been found to be highly efficient for removal of hydrogen concentration in the range of 1.5 to 7.0% v/v in air. Though both the catalysts exhibit similar kinetics for lower hydrogen concentration, cordierite supported catalysts exhibits better kinetic rate at higher hydrogen concentration. The performances of these catalysts in presence of various probable catalytic poison like carbon monoxide and catalytic inhibitors like moisture, carbon dioxide, and hydrocarbons provide data for use of these catalysts under the actual scenario. Compared to stainless steel wire gauze supported catalyst, the cordierite based catalyst are found to exhibit enhanced resistance towards carbon monoxide and limited temperature rise for safer application at higher hydrogen concentrations.

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.

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

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.

Preparation and characterization of multi-walled carbon nanotube (MWCNTs)-supported Pt-Ru catalyst for methanol electrooxidation

Energy Technology Data Exchange (ETDEWEB)

Yang Chunwei [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China)], E-mail: cw.yang@hit.edu.cn; Wang Dianlong; Hu Xinguo; Dai Changsong [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China); Zhang Liang [School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081 (China)

2008-01-10

Multi-walled carbon nanotubes (MWCNTs) as a support of PtRu catalyst nanocomposites were prepared by colloid method in this work. Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) all indicate that ultrasonic treatment can effectively functionalize MWCNTs, endowing them with groups that can act as nucleation sites which can favor well-dispersed deposition of PtRu clusters on their surface. The PtRu/MWCNTs catalysts have a high and homogeneous dispersion of spherical PtRu metal particles with a narrow particle-size distribution. From XPS tests, in PtRu/MWCNTs catalysts Ru can weaken the out-shell electrons of Pt because a part of Ru form alloy with Pt. The remnant Ru exists in oxidation and provides abundant oxygen to nearby Pt, as accelerated desorption and oxidation of intermediate products of methanol oxidation at surface of Pt. By a series of electrochemistry measurements, the PtRu/MWCNTs catalysts display significantly higher performance than the PtRu/XC-72 catalysts. Finally, schematic procedures for the oxidation of MWCNTs and synthesis of PtRu/MWCNTs catalysts were given.

Preparation and characterization of multi-walled carbon nanotube (MWCNTs)-supported Pt-Ru catalyst for methanol electrooxidation

International Nuclear Information System (INIS)

Yang Chunwei; Wang Dianlong; Hu Xinguo; Dai Changsong; Zhang Liang

2008-01-01

Multi-walled carbon nanotubes (MWCNTs) as a support of PtRu catalyst nanocomposites were prepared by colloid method in this work. Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) all indicate that ultrasonic treatment can effectively functionalize MWCNTs, endowing them with groups that can act as nucleation sites which can favor well-dispersed deposition of PtRu clusters on their surface. The PtRu/MWCNTs catalysts have a high and homogeneous dispersion of spherical PtRu metal particles with a narrow particle-size distribution. From XPS tests, in PtRu/MWCNTs catalysts Ru can weaken the out-shell electrons of Pt because a part of Ru form alloy with Pt. The remnant Ru exists in oxidation and provides abundant oxygen to nearby Pt, as accelerated desorption and oxidation of intermediate products of methanol oxidation at surface of Pt. By a series of electrochemistry measurements, the PtRu/MWCNTs catalysts display significantly higher performance than the PtRu/XC-72 catalysts. Finally, schematic procedures for the oxidation of MWCNTs and synthesis of PtRu/MWCNTs catalysts were given

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

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

Electrically conductive aluminum oxide thin film used as cobalt catalyst-support layer in vertically aligned carbon nanotube growth

International Nuclear Information System (INIS)

Azam, Mohd Asyadi; Ismail, Syahriza; Mohamad, Noraiham; Isomura, Kazuki; Shimoda, Tatsuya

2015-01-01

This paper will present the unique characteristics of aluminum oxide (Al–O) and cobalt catalyst included in aligned carbon nanotube (CNT) electrode system of energy storage device, namely electrochemical capacitor. Electrical conductivity and nanostructure of the thermally oxidized Al–O used as catalyst-support layer in vertically grown single-walled CNTs were studied. Al–O films were characterized by means of current–voltage measurement and high resolution transmission electron microscopy analysis. The Al–O support layer was found to be conductive, with a relatively low resistance and, approximately 20 nm film thickness of Al–O is suggested to be too thin to form insulating barrier. The scanning TEM—annular dark field analysis confirmed that the nanosized cobalt catalyst particles distributed on Al–O surfaces and also embedded inside the Al–O film structure. (paper)

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

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

Carbon nanofibers: a versatile catalytic support

Directory of Open Access Journals (Sweden)

Nelize Maria de Almeida Coelho

2008-09-01

Full Text Available The aim of this article is present an overview of the promising results obtained while using carbon nanofibers based composites as catalyst support for different practical applications: hydrazine decomposition, styrene synthesis, direct oxidation of H2S into elementary sulfur and as fuel-cell electrodes. We have also discussed some prospects of the use of these new materials in total combustion of methane and in ammonia decomposition. The macroscopic carbon nanofibers based composites were prepared by the CVD method (Carbon Vapor Deposition employing a gaseous mixture of hydrogen and ethane. The results showed a high catalytic activity and selectivity in comparison to the traditional catalysts employed in these reactions. The fact was attributed, mainly, to the morphology and the high external surface of the catalyst support.

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)

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.

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

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.

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

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.

Life Support Catalyst Regeneration Using Ionic Liquids and In Situ Resources

Science.gov (United States)

Abney, Morgan B.; Karr, Laurel; Paley, Mark S.; Donovan, David N.

2016-01-01

Oxygen recovery from metabolic carbon dioxide is an enabling capability for long-duration manned space flight. Complete recovery of oxygen (100%) involves the production of solid carbon. Catalytic approaches for this purpose, such as Bosch technology, have been limited in trade analyses due in part to the mass penalty for high catalyst resupply caused by carbon fouling of the iron or nickel catalyst. In an effort to mitigate this challenge, several technology approaches have been proposed. These approaches have included methods to prolong the life of the catalysts by increasing the total carbon mass loading per mass catalyst, methods for simplified catalyst introduction and removal to limit the resupply container mass, methods of using in situ resources, and methods to regenerate catalyst material. Research and development into these methods is ongoing, but only use of in situ resources and/or complete regeneration of catalyst material has the potential to entirely eliminate the need for resupply. The use of ionic liquids provides an opportunity to combine these methods in a technology approach designed to eliminate the need for resupply of oxygen recovery catalyst. Here we describe the results of an initial feasibility study using ionic liquids and in situ resources for life support catalyst regeneration, we discuss the key challenges with the approach, and we propose future efforts to advance the technology.

THE THEORY OF DEVELOPMENT OF SUPPORTED METAL-COMPLEX CATALYSTS

Directory of Open Access Journals (Sweden)

T. L. Rakitskaya

2015-06-01

Full Text Available Some results of the investigations for the purpose of development of supported metal-complex catalysts for phosphine and carbon monoxide oxidation as well as for ozone decomposition are summarized. The activity of such catalysts has been found to depend not only on a nature of a central atom and ligands but also on a nature of supports. The theoretical model explaining mechanisms of surface complex formation taking into account the influence of physicochemical and structural-adsorption properties of the supports (SiO2, Al2O3, carbon materials, zeolites, dispersed silicas, lamellar aluminosilicates, etc. has been proposed. For quantitative description of the support effect, such a thermodynamic parameter as the adsorbed water activity assignable with the help of water vapor adsorption isotherms has been introduced. Successive stability constants of the surface metal complexes have been calculated by the kinetic method and, hence, compositions and partial catalytic activity of the latter have been determined. Taking into account the competitive adsorption of metal ions on the supports, some schemes of formation of surface bimetallic complexes have been suggested. The compositions of the supported metal-complex catalysts have been optimized to meet requirements of their use in respirators and plants for air purification from foregoing gaseous toxicants.

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.

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

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.

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.

Basic metal carbonate supported gold nanoparticles: enhanced performance in aerobic alcohol oxidation

NARCIS (Netherlands)

Yang, J.; Guan, Y.; Verhoeven, M.W.G.M.; Santen, van R.A.; Li, Can; Hensen, E.J.M.

2009-01-01

Gold nanoparticles supported by basic hydrozincite or bismuth carbonate are excellent catalysts for liquid-phase aerobic alcohol oxidation: the performance of a series of metal (Zn, Bi, Ce, La, Zr) carbonate supported gold catalysts depends strongly on the basicity of the support material.

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

International Nuclear Information System (INIS)

Wojcieszak, R.

2006-06-01

We have studied Ni or NiAg nano-particles obtained by the reduction of nickel salts (acetate or nitrate) by hydrazine and deposited by simple or EDTA-double impregnation on various supports (γ-Al 2 O 3 , amorphous or crystallized SiO 2 , Nb 2 O 5 , CeO 2 and carbon). Prepared catalysts were characterized by different methods (XRD, XPS, low temperature adsorption and desorption of N 2 , FTIR and FTIR-Pyridine, TEM, STEM, EDS, H 2 -TPR, H 2 -adsorption, H 2 -TPD, isopropanol decomposition) and tested in the gas phase hydrogenation of benzene or as carbon materials in the hydrogen storage at room temperature and high pressure. The catalysts prepared exhibited better dispersion and activity than classical catalysts. TOF's of NiAg/SiO 2 or Ni/carbon catalysts were similar to Pt catalysts in benzene hydrogenation. Differences in support acidity or preparation method and presence of Ag as metal additive play a crucial role in the chemical reduction of Ni by hydrazine and in the final properties of the materials. Ni/carbon catalysts could store significant amounts of hydrogen at room temperature and high pressure (0.53%/30 bars), probably through the hydrogen spillover effect. (author)

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.

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)

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, (O_c)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 MoO_x Tmax of reduction reported to date, suggesting a highly reactive MoVI center. (O_c)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. (O_c)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.

Ni catalysts with different promoters supported on zeolite for dry reforming of methane

KAUST Repository

Alotaibi, Raja; Alenazey, Feraih; Alotaibi, Faisal; Wei, Nini; Al-Fatesh, Ahmed; Fakeeha, Anis

2015-01-01

Dry reforming of methane (DRM) is considered a high endothermic reaction with operating temperatures between 700 and 1000 °C to achieve high equilibrium conversion of CH4 and CO2 to the syngas (H2 and CO). The conventional catalysts used for DRM are Ni-based catalysts. However, many of these catalysts suffer from the short longevity due to carbon deposition. This study aims to evaluate the effect of La and Ca as promoters for Ni-based catalysts supported on two different zeolite supports, ZL (A) (BET surface area = 925 m2/g, SiO2/Al2O3 mol ratio = 5.1), and ZL (B) (BET surface area = 730 m2/g, SiO2/Al2O3 mol ratio = 12), for DRM. The physicochemical properties of the prepared catalysts were characterized with XRD, BET, TEM and TGA. These catalysts were tested for DRM in a microtubular reactor at reaction conditions of 700 °C. The catalyst activity results show that the catalysts Ni/ZL (B) and Ca-Ni/ZL (B) give the highest methane conversion (60 %) with less time on stream stability compared with promoted Ni on ZL (A). In contrast, La-containing catalysts, La-Ni/ZL (B), show more time on stream stability with minimum carbon content for the spent catalyst indicating the enhancement of the promoters to the Ni/ZL (A) and (B), but with less catalytic activity performance in terms of methane and carbon dioxide conversions due to rapid catalyst deactivation.

Ni catalysts with different promoters supported on zeolite for dry reforming of methane

KAUST Repository

Alotaibi, Raja

2015-07-08

Dry reforming of methane (DRM) is considered a high endothermic reaction with operating temperatures between 700 and 1000 °C to achieve high equilibrium conversion of CH4 and CO2 to the syngas (H2 and CO). The conventional catalysts used for DRM are Ni-based catalysts. However, many of these catalysts suffer from the short longevity due to carbon deposition. This study aims to evaluate the effect of La and Ca as promoters for Ni-based catalysts supported on two different zeolite supports, ZL (A) (BET surface area = 925 m2/g, SiO2/Al2O3 mol ratio = 5.1), and ZL (B) (BET surface area = 730 m2/g, SiO2/Al2O3 mol ratio = 12), for DRM. The physicochemical properties of the prepared catalysts were characterized with XRD, BET, TEM and TGA. These catalysts were tested for DRM in a microtubular reactor at reaction conditions of 700 °C. The catalyst activity results show that the catalysts Ni/ZL (B) and Ca-Ni/ZL (B) give the highest methane conversion (60 %) with less time on stream stability compared with promoted Ni on ZL (A). In contrast, La-containing catalysts, La-Ni/ZL (B), show more time on stream stability with minimum carbon content for the spent catalyst indicating the enhancement of the promoters to the Ni/ZL (A) and (B), but with less catalytic activity performance in terms of methane and carbon dioxide conversions due to rapid catalyst deactivation.

Adsorption and desorption of hydrogen and carbon monoxide were studied on alumina-supported iridium catalysts

Energy Technology Data Exchange (ETDEWEB)

Etherton, B.P.

1980-01-01

The adsorption and desorption of hydrogen and carbon monoxide were studied on alumina-supported iridium catalysts which were examined by a scanning transmission electron microscope (STEM). The metal particle size and number of particles per area of catalyst increased with increasing metal loading. The particles were approx. 10 A. in diameter, cubo-octahedral shaped, and approx. 80-90% disperse. The STEM electron beam caused negligible damage to the samples. Hydrogen adsorption measurements showed that the hydrogen-iridium atom ratio was 1.2:1-1.3:1 and increased with decreasing metal loading. Temperature-programed desorption showed four types of adsorbed hydrogen desorbing at -90/sup 0/C (I), 15/sup 0/C (IV), 115/sup 0/C (II), and 245/sup 0/C (III). Types II and IV desorb from single atom sites and Types I and III from multiple atom sites. Type I is in rapid equilibrium with the gas phase. All desorption processes appear to be first order. Carbon monoxide adsorbed nondissociatively at 25/sup 0/C with approx. 0.7:1 CO/Ir atom ratio. It adsorbed primarily in linear forms at low coverage, but a bridged form appeared at high coverage.

SELECTIVE HYDROGENATION OF CINNAMALDEHYDE WITH Pt AND Pt-Fe CATALYSTS: EFFECTS OF THE SUPPORT

Directory of Open Access Journals (Sweden)

A.B. da Silva

1998-06-01

Full Text Available Low-temperature reduced TiO2-supported Pt and Pt-Fe catalysts are much more active and selective for the liquid–phase hydrogenation of cinnamaldehyde to unsaturated cinnamyl alcohol than the corresponding carbon-supported catalysts. High-temperature reduced catalysts, where the SMSI effect should be present, are almost inactive for this reaction. There is at present no definitive explanation for this effect but an electronic metal-support interaction is most probably involved.

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.

An efficient fabrication of vertically aligned carbon nanotubes on flexible aluminum foils by catalyst-supported chemical vapor deposition

International Nuclear Information System (INIS)

Yoshikawa, Naoki; Kishi, Naoki; Sugai, Toshiki; Shinohara, Hisanori; Asari, Takuma; Hayashi, Shigeo

2008-01-01

An efficient and versatile growth of thin-layer carbon nanotubes on a flexible aluminum foil (for kitchen use) by catalyst-supported chemical vapor deposition is reported. The aluminum foil used in the present experiment is commercially available for kitchen use. The electron-beam vapor deposition and dip-coating have been used for preparing catalysts on the aluminum foil. Vertically aligned thin-layer CNTs with typical diameters of 2.5-6.0 nm and lengths up to 90 μm are obtained when ethanol is used in combination with Fe and Co catalyst particles at a growth temperature of around 650 deg. C under an Ar/H 2 gas flow. Thermo-gravimetric analyses together with HR-TEM observations indicate that the purity of the CNTs synthesized by the current technique is very high

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.

Selective production of oxygenates from CO2 hydrogenation over mesoporous silica supported Cu-Ga nanocomposite catalyst

KAUST Repository

Huang, Kuo-Wei; Hengne, Amol Mahalingappa; Bhatte, Kushal Deepak; Ould-Chikh, Samy; Saih, Youssef; Basset, Jean-Marie

2017-01-01

Carbon dioxide hydrogenation to oxygenates (methanol and dimethyl ether (DME)) was investigated over bifunctional supported copper catalysts promoted with gallium (Ga). Supported Cu-Ga nanocomposite catalysts were characterized by X-ray diffraction

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

Hydrous titanium oxide-supported catalysts

International Nuclear Information System (INIS)

Dosch, R.G.; Stohl, F.V.; Richardson, J.T.

1990-01-01

Catalysts were prepared on hydrous titanium oxide (HTO) supports by ion exchange of an active metal for Na + ions incorporated in the HTO support during preparation by reaction with the parent Ti alkoxide. Strong active metal-HTO interactions as a result of the ion exchange reaction can require significantly different conditions for activation as compared to catalysts prepared by more widely used incipient wetness methods. The latter catalysts typically involve conversion or while the HTO catalysts require the alteration of electrostatic bonds between the metal and support with subsequent alteration of the support itself. In this paper, the authors discuss the activation, via sulfidation or reduction, of catalysts consisting of Co, Mo, or Ni-Mo dispersed on HTO supports by ion exchange. Correlations between the activation process and the hydrogenation, hydrodeoxygenation, and hydrodesulfurization activities of the catalysts are presented

A comparison of alumina, carbon and carbon-covered alumina as support for Ni-Mo-F additives: gas oil hydroprocessing studies

Energy Technology Data Exchange (ETDEWEB)

Boorman, P.M.; Kydd, R.A.; Sorensen, T.S.; Chong, K.; Lewis, J.M.; Bell, W.S. (University of Calgary, Calgary, AB (Canada). Dept. of Chemistry)

1991-01-01

Catalysts with 3 wt% NiO, 15 wt% MoO{sub 3} and 0-6.9 nominal wt% fluoride supported on alumina, carbon and carbon-covered alumina were studied to examine the role of fluoride and the influence of the support on hydroprocessing on Alberta gas oil. Experiments were carried out in a batch reactor at 410{degree}C and 6.9 MPa initial H{sub 2} pressure. It was found that fluoride promotion enhances cracking and hydrogenation reactions resulting in decreased aromatic and sulphur contents in the gas oil. The promotion is dependent on the type of support and is related to the strength of the fluoride-support interaction and the accessibility of the fluoride to the surface hydroxyl groups on the support. A maximum in activity at 3.6 wt% fluoride was observed for the alumina-supported catalysts whereas higher loadings of fluoride were required for carbon-covered alumina-supported catalysts to see an improvement over their carbon-supported counterparts. However, the carbon-covered alumina-supported catalysts seem to have a lower propensity for coke deposition than their alumina counterparts. 27 refs., 1 fig., 4 tabs.

A comparison of alumina, carbon and carbon-covered alumina as supports for Ni-Mo-F additives: gas oil hydroprocessing studies

Energy Technology Data Exchange (ETDEWEB)

Boorman, P.M.; Kydd, R.A.; Sorensen, T.S.; Chong, K.; Lewis, J.M.; Bell, W.S. (Calgary Univ., AB (Canada). Dept. of Chemistry)

1992-01-01

Catalysts with 3 wt% NiO, 15 wt% MoO{sub 3} and 0-6.9 nominal wt% fluoride supported on alumina, carbon and carbon-covered alumina were studied to examine the role of fluoride and the influence of the support on hydroprocessing on Alberta gas oil. Experiments were carried out in a batch reactor at 410{sup o}C and 6.9 MPa initial H{sub 2} pressure. It was found that fluoride promotion enhances cracking and hydrogenation reactions resulting in decreased aromatic and sulphur contents in the gas oil. The promotion is dependent on the type of support and is related to the strength of the fluoride-support interaction and the accessibility of the fluoride to the surface hydroxyl groups on the support. A maximum in activity at 3.6 wt% fluoride was observed for the alumina-supported catalysts whereas higher loadings of fluoride were required for carbon-covered alumina-supported catalysts to see an improvement over their carbon supported counterparts. However, the carbon-covered alumina supported catalysts seem to have a lower propensity for coke deposition than their alumina counterparts. (author).

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.

Biotemplated Palladium Catalysts Can Be Stabilized on Different Support Materials

KAUST Repository

Yates, Matthew D.; Logan, Bruce E.

2014-01-01

© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. Sustainably biotemplated palladium catalysts generated on different carbon-based support materials are examined for durability under electrochemical (oxidative) and mechanical-stress conditions. Biotemplated catalysts on carbon paper under both stresses retain 95% (at 0.6V) of the initial catalytic activity as opposed to 70% for carbon cloth and 60% for graphite. Graphite electrodes retain 95% of initial catalytic activity under a single stress. Using electrodeposited polyaniline (PANI) and polydimethylsiloxane binder increases the current density after the stress tests by 22%, as opposed to a 30% decrease for Nafion. PANI-coated electrodes retain more activity than carbon-paper electrodes under elevated mechanical (94 versus 70%) or increased oxidative (175 versus 62%) stress. Biotemplated catalytic electrodes may be useful alternatives to synthetically produce catalysts for some electrochemical applications. Sustainable electrode fabrication: The biotemplated synthesis of catalytic porous electrodes is a sustainable process and, according to the results of durability tests under electrochemical and mechanical stress, these electrodes (e.g. the Pd/carbon paper electrode shown in the picture) are durable enough to replace catalytic electrodes based on synthetic materials in certain applications.

Biotemplated Palladium Catalysts Can Be Stabilized on Different Support Materials

KAUST Repository

Yates, Matthew D.

2014-07-30

© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. Sustainably biotemplated palladium catalysts generated on different carbon-based support materials are examined for durability under electrochemical (oxidative) and mechanical-stress conditions. Biotemplated catalysts on carbon paper under both stresses retain 95% (at 0.6V) of the initial catalytic activity as opposed to 70% for carbon cloth and 60% for graphite. Graphite electrodes retain 95% of initial catalytic activity under a single stress. Using electrodeposited polyaniline (PANI) and polydimethylsiloxane binder increases the current density after the stress tests by 22%, as opposed to a 30% decrease for Nafion. PANI-coated electrodes retain more activity than carbon-paper electrodes under elevated mechanical (94 versus 70%) or increased oxidative (175 versus 62%) stress. Biotemplated catalytic electrodes may be useful alternatives to synthetically produce catalysts for some electrochemical applications. Sustainable electrode fabrication: The biotemplated synthesis of catalytic porous electrodes is a sustainable process and, according to the results of durability tests under electrochemical and mechanical stress, these electrodes (e.g. the Pd/carbon paper electrode shown in the picture) are durable enough to replace catalytic electrodes based on synthetic materials in certain applications.

Cobalt supported on carbon nanofibers as catalysts for the Fischer-Tropsch synthesis

NARCIS (Netherlands)

Bezemer, G.L.

2006-01-01

The Fischer-Tropsch (FT) process converts synthesis gas (H2/CO) over a heterogeneous catalyst into hydrocarbons. Generally, cobalt catalysts supported on oxidic carriers are used for the FT process, however it appears to be difficult to obtain and maintain fully reduced cobalt particles. To overcome

MoP nanoparticles supported on indium-doped porous carbon. Outstanding catalysts for highly efficient CO{sub 2} electroreduction

Energy Technology Data Exchange (ETDEWEB)

Sun, Xiaofu; Lu, Lu; Yang, Dexin; Chen, Chunjun; Han, Buxing [Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Institute of Chemistry Chinese Academy of Sciences, Beijing (China); University of Chinese Academy of Sciences, Beijing (China); Zhu, Qinggong; Wu, Congyi [Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Institute of Chemistry Chinese Academy of Sciences, Beijing (China)

2018-02-23

Electrochemical reduction of CO{sub 2} into value-added product is an interesting area. MoP nanoparticles supported on porous carbon were synthesized using metal-organic frameworks as the carbon precursor, and initial work on CO{sub 2} electroreduction using the MoP-based catalyst were carried out. It was discovered that MoP nanoparticles supported on In-doped porous carbon had outstanding performance for CO{sub 2} reduction to formic acid. The Faradaic efficiency and current density could reach 96.5 % and 43.8 mA cm{sup -2}, respectively, when using ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate as the supporting electrolyte. The current density is higher than those reported up to date with very high Faradaic efficiency. The MoP nanoparticles and the doped In{sub 2}O{sub 3} cooperated very well in catalyzing the CO{sub 2} electroreduction. (copyright 2018 Wiley-VCH Verlag GmbH and Co. KGaA, Weinheim)

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

An iron-57 Moessbauer spectroscopic study of titania-supported iron- and iron-iridium catalysts

International Nuclear Information System (INIS)

Berry, F.J.; Jobson, S.

1992-01-01

57 Fe Moessbauer spectroscopy shows that titania-supported iron is reduced by treatment in hydrogen at significantly lower temperatures than corresponding silica- and alumina-supported catalysts. The metallic iron formed under hydrogen at 600deg C is partially converted to carbide by treatment in carbon monoxide and hydrogen. In contrast to its alumina- and silica-supported counterparts, the remainder of the titania-supported iron is unchanged by this gaseous mixture. The 57 Fe Moessbauer spectra of EXAFS show that iron and iridium in the titania-supported iron-iridium catalysts are reduced in hydrogen at even lower temperatures and, after treatment at 600deg C, are predominantly present as the iron-iridium alloy. The treatment of these reduced catalysts in carbon monoxide and hydrogen is shown by Moessbauer spectroscopy and EXAFS to induce the segregation of iron from the iron-iridium alloy and its conversion to iron oxide. (orig.)

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  |  

Preparation of supported electrocatalyst comprising multiwalled carbon nanotubes

Science.gov (United States)

Wu, Gang; Zelenay, Piotr

2013-08-27

A process for preparing a durable non-precious metal oxygen reduction electrocatalyst involves heat treatment of a ball-milled mixture of polyaniline and multiwalled carbon nanotubes in the presence of a Fe species. The catalyst is more durable than catalysts that use carbon black supports. Performance degradation was minimal or absent after 500 hours of operation at constant cell voltage of 0.40 V.

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

The challenges of treating high strength wastewaters: CWAO using MWNT supported ruthenium catalysts

International Nuclear Information System (INIS)

GarcIa, J.; Gomes, H.T.; Figueiredo, J.L.; Faria, J.L.; Garcia, J.; Serp, P.; Kalck, P.

2005-01-01

High strength wastewaters containing aromatic compounds are normally not efficiently treated by conventional methods, including the common biological treatment. In these cases a more sophisticated approach is necessary to attain the desired levels of purification. Catalytic wet air oxidation (CWAO) using carbon based catalysts is employed worldwide as effective pre-treatment of effluents with these characteristics. Carbon materials are preferred as active catalysts or support for preparing them due to their morphological and structural characteristics. In the last 10 years, due to a tremendous development in materials production and processing, carbon nano-structures are becoming more accessible and common widening their range of applications [1]. In this context, the scope of the present work is to illustrate a potential use of multi-walled carbon nano-tubes (MWNT) supported ruthenium catalysts for catalytic wet air oxidation of aniline polluted wastewaters. The metal was supported by incipient wetness and excess impregnation, starting from liquid solutions of three different Ru precursors. Impregnation was carried out on modified MWNT, namely on MWNT-COOH (HNO 3 modified) and MWNT-COONa (HNO 3 /Na 2 CO 3 modified). For the 1% weight Ru/MWNT catalysts, the order of activities decreased in the sequence Ru(COD)(COT)≥RuCl 3 ≥Ru(C 5 H 5 ) 2 . The conversion of aniline after 45 min of reaction was 100% for the catalyst prepared with Ru(COD)(COT). The influence of the Ru precursor, preparation method and the support surface modification was studied comparing the conversion of aniline obtained for the different prepared Ru/MWNT catalysts (Figure 1). MWNT as support material, provide a significant metal dispersion with very small Ru nanoparticles (Figure 2) being observed. This will induce an efficient surface contact between the aniline molecule and the active sites [2]. The excellent catalytic performances of Ru/MWNT are explained in terms of the high dispersion of

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.

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

A Comparative Study of the Effect of MgO and CaCO3 as Support Materials in the Synthesis of Carbon Nanotubes with Fe/Co as Catalyst

Directory of Open Access Journals (Sweden)

Ezekiel D. Dikio

2014-01-01

Full Text Available A comparative study of the effect of magnesium oxide and calcium carbonate as support material in the synthesis of carbon nanotubes using the catalyst Fe/Co is presented. The synthesized carbon nanotubes were characterized with Raman spectroscopy, scanning electron spectroscopy (SEM, high-resolution transmission electron microscopy (HRTEM, X-ray diffraction spectroscopy (XRD, and energy dispersive spectroscopy (EDS. The morphology of the carbon nanotubes synthesized with magnesium oxide as support material gives rise to carbon nanotubes with consistent and well-defined structure unlike that synthesized with calcium carbonate. The ID/IG ratio of synthesized carbon nanotubes (CNTs was 0.8544 for magnesium oxide supported compared to 0.8501 for calcium carbonate supported carbon nanotube.

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.

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.

Gas-phase Dehydration of Glycerol over Supported Silicotungstic Acids Catalysts

International Nuclear Information System (INIS)

Kim, Yong Tae; Park, Eun Duck; Jung, Kwang Deog

2010-01-01

The gas-phase dehydration of glycerol to acrolein was carried out over 10 wt % HSiW catalysts supported on different supports, viz. γ-Al 2 O 3 , SiO 2 -Al 2 O 3 , TiO 2 , ZrO 2 , SiO 2 , AC, CeO 2 and MgO. The same reaction was also conducted over each support without HSiW for comparison. Several characterization techniques, N 2 -physisorption, thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), the temperature-programmed desorption of ammonia (NH 3 - TPD), temperature-programmed oxidation (TPO) with mass spectroscopy and CHNS analysis were employed to characterize the catalysts. The glycerol conversion generally increased with increasing amount of acid sites. Ceria showed the highest 1-hydroxyacetone selectivity at 315 .deg. C among the various metal oxides. The supported HSiW catalyst showed superior catalytic activity to that of the corresponding support. Among the supported HSiW catalysts, HSiW/ZrO 2 and HSiW/SiO 2 -Al 2 O 3 showed the highest acrolein selectivity. In the case of HSiW/ZrO 2 , the initial catalytic activity was recovered after the removal of the accumulated carbon species at 550 .deg. C in the presence of oxygen

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.

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...

Graphene supported heterogeneous catalysts for Li–O{sub 2} batteries

Energy Technology Data Exchange (ETDEWEB)

Alaf, M., E-mail: mirac.alaf@bilecik.edu.tr [Bilecik Seyh Edebali University, Engineering Faculty, Department of Metallurgy and Materials Engineering, Gulumbe Campus, Bilecik 11210 (Turkey); Tocoglu, U.; Kartal, M.; Akbulut, H. [Sakarya University, Engineering Faculty, Department of Metallurgy and Materials Engineering, Esentepe Campus, Sakarya 54187 (Turkey)

2016-09-01

Graphical abstract: - Highlights: • Free-standing and flexible electrodes were prepared for Li–air batteries. • α-MnO{sub 2} nanorods, Pt nanoparticles and graphene were used. • α-MnO{sub 2} and Pt catalyst improved OER/ORR kinetics. - Abstract: In this study production and characterization of free-standing and flexible (i) graphene, (ii) α-MnO{sub 2}/graphene, (iii) Pt/graphene (iv) α-MnO{sub 2}/Pt/graphene composite cathodes for Li–air batteries were reported. Graphene supported heterogeneous catalysts were produced by a facile method. In order to prevent aggregation of graphene sheets and increase not only interlayer distance but also surface area, a trace amount multi-wall carbon nano tube (MWCNT) was introduced to the composite structure. The obtained composite catalysts were characterized by SEM, X-ray diffraction, N{sub 2} adsorption–desorption analyze and Raman spectroscopy. The electrochemical characterization tests including galvanostatic charge/discharge and electrochemical impedance spectroscopy (EIS) measurement of catalyst were carried out by using an ECC-Air test cell. These highly active graphene supported heterogeneous composite catalysts provide competitive properties relative to other catalyst materials for Li–air batteries.

Study on purification of carbon nano tubes grown on Fe/Ni bimetallic catalyst supported on Mg O by thermal chemical vapor deposition

International Nuclear Information System (INIS)

Mirershadi, S.; Mortazavi, Z.; Reyhani, A.; Norouzian, Sh.; Moniri, N.; Novinrooz, A. J.

2007-01-01

Carbon nano tubes grown on Fe/Ni bimetallic catalysts supported on Mg O by thermal chemical vapor deposition. Then purification of carbon nano tubes by oxidation under air at atmospheric pressure and acid treatment with HCl, have been studied. The Scanning electron microscopy observation showed impurities with carbon nano tubes. Scanning electron microscopy, XRD, Raman spectroscopy and Thermogravimetric analysis/Differential Scanning Calorimetry techniques have been used to investigate the effect of purification of carbon nano tubes on morphology and structural quality of them. The weight ratio of carbon nano tubes in purified sample re saved to 85/8 %.

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.

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.

Methanol Electro-Oxidation on Pt-Ru Alloy Nanoparticles Supported on Carbon Nanotubes

Directory of Open Access Journals (Sweden)

Yangchuan Xing

2009-09-01

Full Text Available Carbon nanotubes (CNTs have been investigated in recent years as a catalyst support for proton exchange membrane fuel cells. Improved catalyst activities were observed and attributed to metal-support interactions. We report a study on the kinetics of methanol electro-oxidation on CNT supported Pt-Ru alloy nanoparticles. Alloy catalysts with different compositions, Pt53Ru47/CNT, Pt69Ru31/CNT and Pt77Ru23/CNT, were prepared and investigated in detail. Experiments were conducted at various temperatures, electrode potentials, and methanol concentrations. It was found that the reaction order of methanol electro-oxidation on the PtRu/CNT catalysts was consistent with what has been reported for PtRu alloys with a value of 0.5 in methanol concentrations. However, the electro-oxidation reaction on the PtRu/CNT catalysts displayed much lower activation energies than that on the Pt-Ru alloy catalysts unsupported or supported on carbon black (PtRu/CB. This study provides an overall kinetic evaluation of the PtRu/CNT catalysts and further demonstrates the beneficial role of CNTs.

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.

The challenges of treating high strength wastewaters: CWAO using MWNT supported ruthenium catalysts

Energy Technology Data Exchange (ETDEWEB)

GarcIa, J.; Gomes, H.T.; Figueiredo, J.L.; Faria, J.L. [Porto Univ., Lab. de Catalise e Materiais, Dept. de Engenharia Quimica, Faculdade de Engenharia (Portugal); Garcia, J. [Madrid Univ. Complutense, Grupo de Catalisis y Operaciones de Separacion, Dept. de Ingenieria Quimica, Facultad de Ciencias (Spain); Serp, P.; Kalck, P. [Ecole Nationale Superieure des Ingenieurs en Arts Chimiques et Technologiques, Lab. de Catalyse, Chimie Fine et Polymeres, 31 - Toulouse (France)

2005-07-01

High strength wastewaters containing aromatic compounds are normally not efficiently treated by conventional methods, including the common biological treatment. In these cases a more sophisticated approach is necessary to attain the desired levels of purification. Catalytic wet air oxidation (CWAO) using carbon based catalysts is employed worldwide as effective pre-treatment of effluents with these characteristics. Carbon materials are preferred as active catalysts or support for preparing them due to their morphological and structural characteristics. In the last 10 years, due to a tremendous development in materials production and processing, carbon nano-structures are becoming more accessible and common widening their range of applications [1]. In this context, the scope of the present work is to illustrate a potential use of multi-walled carbon nano-tubes (MWNT) supported ruthenium catalysts for catalytic wet air oxidation of aniline polluted wastewaters. The metal was supported by incipient wetness and excess impregnation, starting from liquid solutions of three different Ru precursors. Impregnation was carried out on modified MWNT, namely on MWNT-COOH (HNO{sub 3} modified) and MWNT-COONa (HNO{sub 3}/Na{sub 2}CO{sub 3} modified). For the 1% weight Ru/MWNT catalysts, the order of activities decreased in the sequence Ru(COD)(COT){>=}RuCl{sub 3}{>=}Ru(C{sub 5}H{sub 5}){sub 2}. The conversion of aniline after 45 min of reaction was 100% for the catalyst prepared with Ru(COD)(COT). The influence of the Ru precursor, preparation method and the support surface modification was studied comparing the conversion of aniline obtained for the different prepared Ru/MWNT catalysts (Figure 1). MWNT as support material, provide a significant metal dispersion with very small Ru nanoparticles (Figure 2) being observed. This will induce an efficient surface contact between the aniline molecule and the active sites [2]. The excellent catalytic performances of Ru/MWNT are explained

Support Screening Studies on the Hydrogenation of Levulinic Acid to γ-Valerolactone in Water Using Ru Catalysts

Directory of Open Access Journals (Sweden)

Anna Piskun

2016-08-01

Full Text Available γ-Valerolactone (GVL has been identified as a sustainable platform chemical for the production of carbon-based chemicals. Here we report a screening study on the hydrogenation of levulinic acid (LA to GVL in water using a wide range of ruthenium supported catalysts in a batch set-up (1 wt. % Ru, 90 °C, 45 bar of H2, 2 wt. % catalyst on LA. Eight monometallic catalysts were tested on carbon based(C, carbon nanotubes (CNT and inorganic supports (Al2O3, SiO2, TiO2, ZrO2, Nb2O5 and Beta-12.5. The best result was found for Ru/Beta-12.5 with almost quantitative LA conversion (94% and 66% of GVL yield after 2 h reaction. The remaining product was 4-hydroxypentanoic acid (4-HPA. Catalytic activity for a bimetallic RuPd/TiO2 catalyst was by far lower than for the monometallic Ru catalyst (9% conversion after 2 h. The effects of relevant catalyst properties (average Ru nanoparticle size, Brunauer-Emmett-Teller (BET surface area, micropore area and total acidity on catalyst activity were assessed.

Oxidative desulfurization of synthetic diesel using supported catalysts. Part 3. Support effect on vanadium-based catalysts

Energy Technology Data Exchange (ETDEWEB)

Cedeno-Caero, Luis; Gomez-Bernal, Hilda; Fraustro-Cuevas, Adriana; Guerra-Gomez, Hector D.; Cuevas-Garcia, Rogelio [UNICAT, Facultad de Quimica, Universidad Nacional Autonoma de Mexico, Cd. Universitaria 04510, Mexico D.F. (Mexico)

2008-04-15

Oxidesulfurization (ODS) of benzothiophenic compounds prevailing in diesel was conducted with hydrogen peroxide in presence of various catalysts, using a model diesel and actual diesel fuel. ODS activities of dibenzothiophenes (DBTs) in hexadecane for a series of V{sub 2}O{sub 5} catalysts supported on alumina, titania, ceria, niobia and silica, were evaluated. Results show that the oxidation activity of DBTs depends on the support used. It was observed that the sulfone yield is not proportional to textural properties or V content. For all catalysts, ODS of benzothiophene (BT), dibenzothiophene (DBT), 4-methyl dibenzothiophene (4-MDBT) and 4,6-dimethyl dibenzothiophene (4,6-DMDBT) decreased in the following order: DBT > 4-MDBT > 4,6-DMDBT > BT. This trend does not depend on the catalyst used or the textural properties of the catalysts and supports. In presence of indole ODS activities diminish, except with catalysts supported on alumina-titania mixed oxide, whereas with V{sub 2}O{sub 5}/TiO{sub 2} catalyst the performance is the highest. ODS of Mexican diesel fuel was carried out in presence of this catalyst and S level was diminished in about 99%. (author)

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.

Removal of toluene by sequential adsorption-plasma oxidation: Mixed support and catalyst deactivation.

Science.gov (United States)

Qin, Caihong; Huang, Xuemin; Zhao, Junjie; Huang, Jiayu; Kang, Zhongli; Dang, Xiaoqing

2017-07-15

A sequential adsorption-plasma oxidation system was used to remove toluene from simulated dry air using γ-Al 2 O 3 , HZSM-5, a mixture of the two materials or their supported Mn-Ag catalyst as adsorbents under atmospheric pressure and room temperature. After 120min of plasma oxidation, γ-Al 2 O 3 had a better carbon balance (∼75%) than HZSM-5, but the CO 2 yield of γ-Al 2 O 3 was only ∼50%; and there was some desorption of toluene when γ-Al 2 O 3 was used. When a mixture of HZSM-5 and γ-Al 2 O 3 with a mass ratio of 1/2 was used, the carbon balance was up to 90% and 82% of this was CO 2 . The adsorption performance and electric discharge characteristics of the mixed supports were tested in order to rationalize this high CO x yield. After seven cycles of sequential adsorption-plasma oxidation, support and Mn-Ag catalyst deactivation occurred. The support and catalyst were characterized before and after deactivation by SEM, a BET method, XRD, XPS and GC-MS in order to probe the mechanism of their deactivation. 97.6% of the deactivated supports and 76% of the deactivated catalysts could be recovered by O 2 temperature-programmed oxidation. Copyright © 2017 Elsevier B.V. All rights reserved.

Electrocatalytic properties of graphite nanofibers-supported platinum catalysts for direct methanol fuel cells.

Science.gov (United States)

Park, Soo-Jin; Park, Jeong-Min; Seo, Min-Kang

2009-09-01

Graphite nanofibers (GNFs) treated at various temperatures were used as carbon supports to improve the efficiency of PtRu catalysts. The electrochemical properties of the PtRu/GNFs catalysts were then investigated to evaluate their potential for application in DMFCs. The results indicated that the particle size and dispersibility of PtRu in the catalysts were changed by heat treatment, and the electrochemical activity of the catalysts was improved. Consequently, it was found that heat treatments could have an influence on the surface and structural properties of GNFs, resulting in enhancing an electrocatalytic activity of the catalysts for DMFCs.

Synthesis of carbon nanotubes by CVD method using iron and molybdenum-based catalysts supported on ceramic matrices

International Nuclear Information System (INIS)

Teixeira, Ana Paula de Carvalho

2010-01-01

Molybdenum is known for its synergistic effect in the synthesis of carbon nanotubes (CNs) by chemical vapor deposition (CVD method). When added to typical catalysts like iron, nickel, and cobalt, even in small quantities, it is increases the yield of these nanostructures. The presence of Mo also has an influence on the type and number of CN walls formed. Although this effect is widely documented in the literature, there is not yet a consensus about the mechanism of action of molybdenum in catalytic systems. The objective of the present work is to study the influence of molybdenum on the catalytic activity of iron nanoparticle-based catalysts supported on magnesium oxide (Fe/MgO system) in the synthesis of carbon nanotubes by the CVD method. The Mo concentration was systematically varied from null to molar ratio values four times greater than the quantity of Fe, and the obtained material (catalysts and carbon nanotubes) were broadly characterized by different techniques. In order to also study the influence of the preparation method on the final composition of the catalytic system phases, the catalytic systems (Fe/MgO e FeMo x /MgO) were synthesized by two different methods: co-precipitation and impregnation. The greatest CN yields were observed for the catalysts prepared by coprecipitation. The difference was attributed to better dispersion of the Fe and Mo phases in the catalyst ceramic matrix. In the precipitation stage, it was observed the formation of layered double hydroxides whose concentration increased with the Mo content up to the ratio of Mo/Fe equal to 0.2. This phase is related to a better distribution of Fe and Mo in this concentration range. Another important characteristic observed is that the ceramic matrix is not inert. It can react both with Fe and Mo and form the iron solid solution in the magnesium oxide and the phases magnesium-ferrite (MgFe 2 0 4 ) and magnesium molybdate (MgMo0 4 ). The MgFe 2 0 4 phase is observed in all catalytic systems

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.

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.

Impeded solid state reactions and transformations in ceramic catalysts supports and catalysts

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Ernő E. Kiss

2012-12-01

Full Text Available Impeded chemical reactions and impeded polymorphous transformation in materials are discussed, as desired effects, for stabilization of ceramic catalyst supports and ceramic based catalysts. This paper gives a short overview about the possibilities of slowing down the aging processes in ceramic catalyst supports and catalysts. Special attention is given to alumina and titania based catalysts.

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

CTAB assisted microwave synthesis of ordered mesoporous carbon supported Pt nanoparticles for hydrogen electro-oxidation

International Nuclear Information System (INIS)

Zhou, Jian-Hua; He, Jian-Ping; Ji, Ya-Jun; Dang, Wang-Juan; Liu, Xiao-Lei; Zhao, Gui-Wang; Zhang, Chuan-Xiang; Zhao, Ji-Shuang; Fu, Qing-Bin; Hu, Huo-Ping

2007-01-01

Mesoporous carbon with ordered hexagonal structure derived from the co-assembly of triblock copolymer F127 and resol was employed as the carbon support of Pt catalysts for hydrogen electro-oxidation. Structural characterizations revealed that the mesoporous carbon exhibited large surface area and uniform mesopores. The Pt nanoparticles supported on the novel mesoporous carbon were fabricated by a facile CTAB assisted microwave synthesis process, wherein CTAB was expected to improve the wettability of carbon support as well as the dispersion of Pt nanoparticles. X-ray diffraction and transmission electron microscopy were applied to characterize the Pt catalysts. It was found that the Pt nanoparticles were uniform in size and highly dispersed on the mesoporous carbon supports. The cyclic voltammograms in sulfuric acid demonstrated that the electrochemical active surface area of Pt catalysts prepared with CTAB was two times than that without CTAB

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

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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.

Preparation of Mesoporous Silica-Supported Palladium Catalysts for Biofuel Upgrade

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Ling Fei

2012-01-01

Full Text Available We report the preparation of two hydrocracking catalysts Pd/CoMoO4/silica and Pd/CNTs/CoMoO4/silica (CNTs, carbon nanotubes. The structure, morphologies, composition, and thermal stability of catalysts were studied by X-ray diffraction (XRD, scanning electron microscopy (SEM, Raman spectroscopy, transmission electron microscopy (TEM, energy-dispersive X-ray (EDX, and thermogravimetric analysis (TGA. The catalyst activity was measured in a Parr reactor with camelina fatty acid methyl esters (FAMEs as the feed. The analysis shows that the palladium nanoparticles have been incorporated onto mesoporous silica in Pd/CoMoO4/silica or on the CNTs surface in Pd/CNTs/CoMoO4/silica catalysts. The different combinations of metals and supports have selective control cracking on heavy hydrocarbons.

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.

The effect of catalyst support on the RWGS reaction

International Nuclear Information System (INIS)

Laosiripojana, N.; Sutthisripok, W.

2004-01-01

'Full text:' Methane steam reforming is generally applied in order to produce synthesis gas mainly consist of hydrogen and carbon monoxide for later utilization in SOFC. This reaction is always carried out with the water gas shift reaction over a catalyst at elevated temperatures resulting in some carbon dioxide production. The CO/CO2 production selectivity strongly depends on the influence of water gas shift reaction. It was observed that the reactivity of this reaction depended on the type of support material. Stabilities, activities, and kinetics of the reverse water gas shift reaction (RWGS) for commercial nickel on CeO2, ZrO2, CeO2-ZrO2, TiO2, MgO, and Al2O3 supports were studied in order to observe the influence of the support on this reaction. According to the experiment, the activities of Ni/CeO2 toward the reverse water gas shift reaction (RWGS) were very high, and reached equilibrium level at approximately 600 o C (where the conversion of CO2 was closed to 1). Other oxide supports provided lower activities toward this reaction. It was observed that the activity of Ni/Al2O3 toward this reaction was the lowest. The kinetics of this reaction was also studied. Carbon dioxide presented positive effect on the reverse water gas shift reaction. The reaction orders in carbon dioxide were observed to be positive partial value between 0-1. It slightly decreased with increasing temperature for Ni/ CeO2 and Ni/CeO2-ZrO2, whereas it seemed to be independent of the operating temperature for other materials in the range of conditions studied. Hydrogen also showed positive effect on the reverse water gas shift reaction for all materials. The reaction order in hydrogen for all materials was observed to be the positive value and less than one for the range of conditions studied. The approximate values for all catalysts were between 0.45-0.65, and seemed to be independent of the operating temperature. The estimated values of the apparent activation energy for RWGS reaction

A Study of CO2 Methanation over Ni-Based Catalysts Supported by CNTs with Various Textural Characteristics

Directory of Open Access Journals (Sweden)

Yanyan Feng

2015-01-01

Full Text Available This work studied the influence of textural characteristics of CNTs on catalytic performance of Ni/CNTs for CO2 methanation. The CNTs supports were prepared by chemical vapor deposition method using Ni/MgO catalysts, and acetonitrile and ethanol were used as carbon sources, respectively. The Ni/CNTs catalysts were prepared via impregnation method and characterized by X-ray diffraction (XRD, N2 adsorption/desorption, and temperature-programmed reduction (H2-TPR techniques. The results indicated that the textural characteristics of CNTs supports significantly impacted on the catalytic performance of Ni/CNTs. The catalyst Ni/CNTs-E (CNTs using ethanol as carbon source had good reducibility, high specific surface area, and moderate defects, resulting in higher CO2 conversion and CH4 yield, followed by Ni/CNTs-C (commercial CNTs and Ni/CNTs-A (CNTs using acetonitrile as carbon source. Based on Arrhenius formula, activation energies of the catalysts were calculated and were found decreased for Ni/CNTs-A and Ni/CNTs-E.

Graphene-oxide-supported CuAl and CoAl layered double hydroxides as enhanced catalysts for carbon-carbon coupling via Ullmann reaction

Science.gov (United States)

Ahmed, Nesreen S.; Menzel, Robert; Wang, Yifan; Garcia-Gallastegui, Ainara; Bawaked, Salem M.; Obaid, Abdullah Y.; Basahel, Sulaiman N.; Mokhtar, Mohamed

2017-02-01

Two efficient catalyst based on CuAl and CoAl layered double hydroxides (LDHs) supported on graphene oxide (GO) for the carbon-carbon coupling (Classic Ullmann Homocoupling Reaction) are reported. The pure and hybrid materials were synthesised by direct precipitation of the LDH nanoparticles onto GO, followed by a chemical, structural and physical characterisation by electron microscopy, X-ray diffraction (XRD), thermogravimetric analysis (TGA), surface area measurements and X-ray photoelectron spectroscopy (XPS). The GO-supported and unsupported CuAl-LDH and CoAl-LDH hybrids were tested over the Classic Ullman Homocoupling Reaction of iodobenzene. In the current study CuAl- and CoAl-LDHs have shown excellent yields (91% and 98%, respectively) at very short reaction times (25 min). GO provides a light-weight, charge complementary and two-dimensional material that interacts effectively with the 2D LDHs, in turn enhancing the stability of LDH. After 5 re-use cycles, the catalytic activity of the LDH/GO hybrid is up to 2 times higher than for the unsupported LDH.

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)

Nitrogen: Unraveling the Secret to Stable Carbon-Supported Pt-Alloy Electrocatalysts

Science.gov (United States)

2013-10-01

release; distribution is unlimited. Nitrogen: unraveling the secret to stable carbon-supported Pt- alloy electrocatalysts The views, opinions and/or...Nitrogen: unraveling the secret to stable carbon-supported Pt-alloy electrocatalysts Report Title Nitrogen functionalities significantly improve...design and optimization of next generation high performance catalyst materials. Nitrogen: unraveling the secret to stable carbon-supported Pt-alloy

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.

Oxidation catalysts on alkaline earth supports

Science.gov (United States)

Mohajeri, Nahid

2017-03-21

An oxidation catalyst includes a support including particles of an alkaline earth salt, and first particles including a palladium compound on the support. The oxidation catalyst can also include precious metal group (PMG) metal particles in addition to the first particles intermixed together on the support. A gas permeable polymer that provides a continuous phase can completely encapsulate the particles and the support. The oxidation catalyst may be used as a gas sensor, where the first particles are chemochromic particles.

Catalytic hydrotreatment of fast pyrolysis oil using bimetallic Ni-Cu catalysts on various supports

NARCIS (Netherlands)

Ardiyanti, A. R.; Khromova, S. A.; Venderbosch, R. H.; Yakovlev, V. A.; Melian-Cabrera, I. V.; Heeres, H. J.

2012-01-01

Bimetallic Ni-Cu catalysts on various Supports (CeO2-ZrO2, ZrO2, SiO2, TiO2, rice husk carbon, and Sibunite) with metal contents ranging from 7.5 to 9.0 (Ni) and 3.1-3.6 wt.% (Cu) for the inorganic supports and 17.1-17.8 (Ni) and 7.1-7.8 (Cu) for the carbon supports were synthesised and screened for

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.

Session 6: Catalytic hydro-dehalogenation of halon 1211 (CBrClF{sub 2}) over carbon supported Pd-Fe, Pd-Co and Pd-Ni bimetallic catalysts

Energy Technology Data Exchange (ETDEWEB)

Hai, Yu; Kennedy, E.M.; Md Azhar, Uddin; Dlugogorski, B.Z. [Newcastle Univ., Process Safety and Environment Protection Group, School of Engineering, Callaghan, NSW (Australia)

2004-07-01

In the current study, we present the result of our investigation on the hydro-dehalogenation of halon 1211 with hydrogen over carbon supported Pd-Fe, Pd-Co and Pd-Ni bimetallic catalysts. In addition to dissociatively adsorbing hydrogen, Fe, Co and Ni themselves can facilitate cleavage of C-halogen bonds. The effect of the interaction of a second metal (Fe, Co and Ni) with Pd on the conversion of halon 1211 and selectivity to CH{sub 2}F{sub 2} for the catalytic hydro-dehalogenation of halon 1211 is discussed. Activated carbon is chosen as support in order to minimize the interaction of support with the metals. The obtained experimental results show that the introduction of Fe, Co and Ni to Pd catalysts has a significant influence on the catalytic hydro-dehalogenation of halon 1211, especially with respect to the selectivity to CH{sub 2}F{sub 2}. The presence of Fe increases the amount of halon 1211 adsorbed on the surface of catalysts and enhances the cleavage of C-halogen bonds in halon 1211, resulting in a higher halon 1211 conversion level and selectivity to hydrocarbons. Higher selectivity to CHBrF{sub 2} is ascribed to the secondary reaction: CF{sub 2} + HBr {yields} CHBrF{sub 2}. (authors)

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 ...

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.)

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.

Hydrothermal performance of catalyst supports

Energy Technology Data Exchange (ETDEWEB)

Elam, Jeffrey W.; Marshall, Christopher L.; Libera, Joseph A.; Dumesic, James A.; Pagan-Torres, Yomaira J.

2018-04-10

A high surface area catalyst with a mesoporous support structure and a thin conformal coating over the surface of the support structure. The high surface area catalyst support is adapted for carrying out a reaction in a reaction environment where the thin conformal coating protects the support structure within the reaction environment. In various embodiments, the support structure is a mesoporous silica catalytic support and the thin conformal coating comprises a layer of metal oxide resistant to the reaction environment which may be a hydrothermal environment.

Understanding the performance and mechanism of Mg-containing oxides as support catalysts in the thermal dry reforming of methane.

Science.gov (United States)

Khairudin, Nor Fazila; Sukri, Mohd Farid Fahmi; Khavarian, Mehrnoush; Mohamed, Abdul Rahman

2018-01-01

Dry reforming of methane (DRM) is one of the more promising methods for syngas (synthetic gas) production and co-utilization of methane and carbon dioxide, which are the main greenhouse gases. Magnesium is commonly applied in a Ni-based catalyst in DRM to improve catalyst performance and inhibit carbon deposition. The aim of this review is to gain better insight into recent developments on the use of Mg as a support or promoter for DRM catalysts. Its high basicity and high thermal stability make Mg suitable for introduction into the highly endothermic reaction of DRM. The introduction of Mg as a support or promoter for Ni-based catalysts allows for good metal dispersion on the catalyst surface, which consequently facilitates high catalytic activity and low catalyst deactivation. The mechanism of DRM and carbon formation and reduction are reviewed. This work further explores how different constraints, such as the synthesis method, metal loading, pretreatment, and operating conditions, influence the dry reforming reactions and product yields. In this review, different strategies for enhancing catalytic activity and the effect of metal dispersion on Mg-containing oxide catalysts are highlighted.

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)

Selective hydrogenation of citral over supported Pt catalysts: insight into support effects

Energy Technology Data Exchange (ETDEWEB)

Wang, Xiaofeng [Missouri University of Science and Technology, Department of Chemical and Biochemical Engineering (United States); Hu, Weiming; Deng, Baolin [University of Missouri, Department of Civil and Environmental Engineering (United States); Liang, Xinhua, E-mail: liangxin@mst.edu [Missouri University of Science and Technology, Department of Chemical and Biochemical Engineering (United States)

2017-04-15

Highly dispersed platinum (Pt) nanoparticles (NPs) were deposited on various substrates by atomic layer deposition (ALD) in a fluidized bed reactor at 300 °C. The substrates included multi-walled carbon nanotubes (MWCNTs), silica gel (SiO{sub 2}), commercial γ-Al{sub 2}O{sub 3}, and ALD-prepared porous Al{sub 2}O{sub 3} particles (ALD-Al{sub 2}O{sub 3}). The results of TEM analysis showed that ~1.3 nm Pt NPs were highly dispersed on all different supports. All catalysts were used for the reaction of selective hydrogenation of citral to unsaturated alcohols (UA), geraniol, and nerol. Both the structure and acidity of supports affected the activity and selectivity of Pt catalysts. Pt/SiO{sub 2} showed the highest activity due to the strong acidity of SiO{sub 2} and the conversion of citral reached 82% after 12 h with a selectivity of 58% of UA. Pt/MWCNTs showed the highest selectivity of UA, which reached 65% with a conversion of 38% due to its unique structure and electronic effect. The cycling experiments indicated that Pt/MWCNTs and Pt/ALD-Al{sub 2}O{sub 3} catalysts were more stable than Pt/SiO{sub 2}, as a result of the different interactions between the Pt NPs and the supports.

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.

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.

Vapor phase carbonylation of dimethyl ether and methyl acetate with supported transition metal catalysts

International Nuclear Information System (INIS)

Shikada, T.; Fujimoto, K.; Tominaga, H.O.

1986-01-01

The synthesis of acetic acid (AcOH) from methanol (MeOH) and carbon monoxide has been performed industrially in the liquid phase using a rhodium complex catalyst and an iodide promoter. The selectivity to AcOH is more than 99% under mild conditions (175 0 C, 28 atm). The homogeneous rhodium catalyst has been also effective for the synthesis of acetic anhydride (Ac 2 O) by carbonylation of dimethyl ether (DME) or methyl acetate (AcOMe). However, rhodium is one of the most expensive metals and its proved reserves are quite limited. It is highly desired, therefore, to develop a new catalyst as a substitute for rhodium. The authors have already reported that nickel supported on active carbon exhibits an excellent activity for the vapor phase carbonylation of MeOh in the presence of iodide promoter and under moderately pressurized conditions. In addition, corrosive attack on reactors by iodide compounds is expected to be negligible in the vapor phase system. In the present work, vapor phase carbonylation of DME and AcOMe on nickel-active carbon (Ni/A.C.) and molybdenum-active carbon (Mo/A.C.) catalysts was studied

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.

Oxidative desulfurization of diesel by potato based-carbon as green support for H5PMo10V2O40: Efficient composite nanorod catalyst

Directory of Open Access Journals (Sweden)

Ezzat Rafiee

2017-07-01

Full Text Available The C@POM (carbon@polyoxometalate containing H3PMo12O40 (PMo12, H5PMo10V2O40 (PMo10V2, H6PMo9V3O40 (PMo9V3, H7PMo8V4O40 (PMo8V4, H3PW12O40 (PW, and H4SiW12O40 (SiW were prepared from natural potato as green, and cheap catalyst support source. The C@PMo10V2 was found to be a unique, effective, and eco-friendly catalyst for selective oxidation of sulfides, using 30% aq. H2O2. C@PMo10V2 composite was characterized by X-ray diffraction spectroscopy (XRD, energy dispersive X-ray spectroscopy (EDX, scanning electron microscopy (SEM, thermal gravimetric analysis (TGA, Fourier transform infrared (FT-IR spectrophotometry, zeta sizer, and zeta potential. The XRD results show that during immobilization PMo10V2 on the carbon catalyst support (CCS, the crystallite structure of PMo10V2 and CCS was not changed. The SEM results show that PMo10V2 crystals deposited on the surface CCS rods as composite nanorod structure. A variety of sulfides, sulfur-containing model and real oil were oxidized with the C@PMo10V2/H2O2 at room temperature. Recovered catalyst show excellent activity for at least four repeating cycles.

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.

The structure of nano-palladium deposited on carbon-based supports

International Nuclear Information System (INIS)

Pikna, Ľubomír; Milkovič, Ondrej; Saksl, Karel; Heželová, Mária; Smrčová, Miroslava; Puliš, Pavel; Michalik, Štefan; Gamcová, Jana

2014-01-01

Nano-palladium catalysts, prepared using the same procedure with the same metal content (3 wt%) and two different supports, activated carbon (Pd/C) and activated carbon—multiwalled carbon nanotubes (Pd/C/CNT), are discussed. The simple technique of deposition reduction was applied in the preparation of these two types of Pd catalysts. TEM, XRD analysis, EXAFS signal analysis, and XANES were used for sample characterization. In both samples, transmission electron microscopy identified nanosized Pd particles with nearly spherical morphology but different sizes. The mean diameters of the particles on Pd/C and Pd/C/CNT were estimated to be 5.4 nm and 7.8 nm, respectively. The EXAFS signal analysis showed that Pd atoms on the particle surfaces were coordinated by 4 oxygens to form a PdO monolayer covering a metallic core. The XANES signal analysis indicated a smaller particle size for Pd/C (∅ 5 nm) than for Pd/C/CNT (∅ 10 nm), in good agreement with the TEM observations. - Graphical abstract: Visualization of metallic core (left), oxide monolayer (middle) and nanoparticle of diameter 5 nm (right). - Highlights: • Pd catalysts were prepared on two types of supports: carbon and carbon nanotubes. • BET, TEM, XRD characterization of prepared catalysts. • XAFS: Concentration of Pd in samples Pd/C and Pd/C/CNT. • EXAFS and XANES signal analysis of catalysts. • Visualisation of atoms arrangement at the Pd nanoparticle surface

Low-temperature carbon monoxide oxidation over zirconia-supported CuO–CeO{sub 2} catalysts: Effect of zirconia support properties

Energy Technology Data Exchange (ETDEWEB)

Moretti, Elisa, E-mail: elisa.moretti@unive.it [Dipartimento di Scienze Molecolari e Nanosistemi, Università Ca' Foscari Venezia, INSTM Venice Research Unit, Via Torino 155/B, 30172 Mestre Venezia (Italy); Molina, Antonia Infantes [Departamento de Química Inorgánica, Cristalografía y Mineralogía, Facultad de Ciencias, Universidad de Málaga, Campus de Teatinos, 29071 Málaga (Spain); Sponchia, Gabriele; Talon, Aldo; Frattini, Romana [Dipartimento di Scienze Molecolari e Nanosistemi, Università Ca' Foscari Venezia, INSTM Venice Research Unit, Via Torino 155/B, 30172 Mestre Venezia (Italy); Rodriguez-Castellon, Enrique [Departamento de Química Inorgánica, Cristalografía y Mineralogía, Facultad de Ciencias, Universidad de Málaga, Campus de Teatinos, 29071 Málaga (Spain); Storaro, Loretta [Dipartimento di Scienze Molecolari e Nanosistemi, Università Ca' Foscari Venezia, INSTM Venice Research Unit, Via Torino 155/B, 30172 Mestre Venezia (Italy)

2017-05-01

Highlights: • CuO-CeO{sub 2}/ZrO{sub 2} materials were investigated in the low temperature CO oxidation. • High surface area ZrO{sub 2} synthetized by sol-gel method. • Low ZrO{sub 2} surface area synthetized by fast precipitation. • Sol-gel samples showed, after impregnation, a severe decrease of surface area. • CuO-CeO{sub 2}/ZrO{sub 2} with precipitated ZrO{sub 2} led to a very active catalyst. - Abstract: A study was conducted to investigate the effect of the preparation route of ZrO{sub 2} in CuO–CeO{sub 2}/ZrO{sub 2} catalysts for the oxidation of carbon monoxide at low temperature (COX). Four ZrO{sub 2} supports were synthetized via either type sol-gel methodology or precipitation. The final Cu-Ce-Zr oxide catalysts were prepared by incipient wetness co-impregnation with copper and cerium solutions (with a loading of 6 wt% of CuO and 20 wt% of CeO{sub 2}). The catalyst crystalline phases, texture and active species reducibility were determined by XRD, N{sub 2} physisorption at −196 °C and H{sub 2}-TPR, respectively; meanwhile the surface composition and copper-cerium electronic states were studied by XPS. The catalytic activity was evaluated in the oxidation of CO to CO{sub 2}, in the 40–215 °C temperature range. Catalytic results evidenced that the samples prepared by a sol-gel methodology showed, after the impregnation, a severe decrease of specific surface area and pore volume attributable to a wide degree of pore blockage caused by the presence of metal oxide particles and a collapse of the structure partially burying the active sites. A simple co-impregnation of a zirconia support, obtained through facile and fast precipitation, provided instead a catalyst with very good redox properties and high dispersion of the active phases, which completely oxidizes CO in the range 115–215 °C with T{sub 50} of 65 °C. This higher observed activity was ascribed to the formation of a larger fraction of highly dispersed and easily reducible Cu

Ethanol electrooxidation on novel carbon supported Pt/SnO{sub x}/C catalysts with varied Pt:Sn ratio

Energy Technology Data Exchange (ETDEWEB)

Jiang, L. [Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm (Germany); Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian (China); Colmenares, L.; Jusys, Z. [Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm (Germany); Sun, G.Q. [Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian (China)], E-mail: gqsun@dicp.ac.cn; Behm, R.J. [Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm (Germany)], E-mail: juergen.behm@uni-ulm.de

2007-12-01

Novel carbon supported Pt/SnO{sub 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{sub ad} stripping) and their electrocatalytic activity and selectivity for ethanol oxidation (ethanol oxidation reaction (EOR)). The data show that the Pt/SnO{sub 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{sub x}/C catalysts towards the EOR decreases with tin content at room temperature, but increases at 80 deg. C. On all Pt/SnO{sub x}/C catalysts, acetic acid and acetaldehyde represent dominant products, CO{sub 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{sup -1}), but are lower than on Pt/C (32 kJ mol{sup -1}). The somewhat better performance of the Pt/SnO{sub x}/C catalysts compared to alloyed PtSn{sub 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.

Fabrication and Characterization of New Composite Tio2 Carbon Nanofiber Anodic Catalyst Support for Direct Methanol Fuel Cell via Electrospinning Method

Science.gov (United States)

Abdullah, N.; Kamarudin, S. K.; Shyuan, L. K.; Karim, N. A.

2017-12-01

Platinum (Pt) is the common catalyst used in a direct methanol fuel cell (DMFC). However, Pt can lead towards catalyst poisoning by carbonaceous species, thus reduces the performance of DMFC. Thus, this study focuses on the fabrication of a new composite TiO2 carbon nanofiber anodic catalyst support for direct methanol fuel cells (DMFCs) via electrospinning technique. The distance between the tip and the collector (DTC) and the flow rate were examined as influencing parameters in the electrospinning technique. To ensure that the best catalytic material is fabricated, the nanofiber underwent several characterizations and electrochemical tests, including FTIR, XRD, FESEM, TEM, and cyclic voltammetry. The results show that D18, fabricated with a flow rate of 0.1 mLhr-1 and DTC of 18 cm, is an ultrafine nanofiber with the smallest average diameter, 136.73 ± 39.56 nm. It presented the highest catalyst activity and electrochemical active surface area value as 274.72 mAmg-1 and 226.75m2 g-1 PtRu, respectively, compared with the other samples.

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.

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.

Influence of silica-alumina support ratio on H2 production and catalyst carbon deposition from the Ni-catalytic pyrolysis/reforming of waste tyres.

Science.gov (United States)

Zhang, Yeshui; Tao, Yongwen; Huang, Jun; Williams, Paul

2017-10-01

The influence of catalyst support alumina-silica in terms of different Al 2 O 3 to SiO 2 mole ratios containing 20 wt.% Ni on the production of hydrogen and catalyst coke formation from the pyrolysis-catalysis of waste tyres is reported. A two-stage reactor system was used with pyrolysis of the tyres followed by catalytic reaction. There was only a small difference in the total gas yield and hydrogen yield by changing the Al 2 O 3 to SiO 2 mole ratios in the Ni-Al 2 O 3 /SiO 2 catalyst. The 1:1 ratio of Al 2 O 3 :SiO 2 ratio produced the highest gas yield of 27.3 wt.% and a hydrogen production of 14.0 mmol g -1 tyre . Catalyst coke formation decreased from 19.0 to 13.0 wt.% as the Al 2 O 3 :SiO 2 ratio was changed from 1:1 to 2:1, with more than 95% of the coke being filamentous-type carbon, a large proportion of which was multi-walled carbon nanotubes. Further experiments introduced steam to the second-stage reactor to investigate hydrogen production for the pyrolysis-catalytic steam reforming of the waste tyres using the 1:1 Al 2 O 3 /SiO 2 nickel catalyst. The introduction of steam produced a marked increase in total gas yield from ~27 wt. % to ~58 wt.%; in addition, hydrogen production was increased to 34.5 mmol g -1 and there was a reduction in catalyst coke formation to 4.6 wt.%.

Influence of silica–alumina support ratio on H2 production and catalyst carbon deposition from the Ni-catalytic pyrolysis/reforming of waste tyres

Science.gov (United States)

Zhang, Yeshui; Tao, Yongwen; Huang, Jun; Williams, Paul

2017-01-01

The influence of catalyst support alumina–silica in terms of different Al2O3 to SiO2 mole ratios containing 20 wt.% Ni on the production of hydrogen and catalyst coke formation from the pyrolysis-catalysis of waste tyres is reported. A two-stage reactor system was used with pyrolysis of the tyres followed by catalytic reaction. There was only a small difference in the total gas yield and hydrogen yield by changing the Al2O3 to SiO2 mole ratios in the Ni-Al2O3/SiO2 catalyst. The 1:1 ratio of Al2O3:SiO2 ratio produced the highest gas yield of 27.3 wt.% and a hydrogen production of 14.0 mmol g-1tyre. Catalyst coke formation decreased from 19.0 to 13.0 wt.% as the Al2O3:SiO2 ratio was changed from 1:1 to 2:1, with more than 95% of the coke being filamentous-type carbon, a large proportion of which was multi-walled carbon nanotubes. Further experiments introduced steam to the second-stage reactor to investigate hydrogen production for the pyrolysis-catalytic steam reforming of the waste tyres using the 1:1 Al2O3/SiO2 nickel catalyst. The introduction of steam produced a marked increase in total gas yield from ~27 wt. % to ~58 wt.%; in addition, hydrogen production was increased to 34.5 mmol g-1 and there was a reduction in catalyst coke formation to 4.6 wt.%. PMID:28789599

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.

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.

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.

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

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.

In-situ hydrodeoxygenation of phenol by supported Ni catalyst-explanation for catalyst performance

DEFF Research Database (Denmark)

Wang, Ze; Zeng, Ying; Lin, Weigang

2017-01-01

In-situ hydrodeoxygenation of phenol with aqueous hydrogen donor over supported Ni catalyst was investigated. The supported Ni catalysts exerted very poor performance, if formic acid was used as the hydrogen donor. Catalyst modification by loading K, Na, Mg or La salt could not make the catalyst...... performance improved. If gaseous hydrogen was used as the hydrogen source the activity of Ni/Al2O3 was pretty high. CO2 was found poisonous to the catalysis, due to the competitive adoption of phenol with CO2. If formic acid was replaced by methanol, the catalyst performance improved remarkably, with major...... products of cyclohexanone and cyclohexanol. The better effect of methanol enlightened the application of the supported Ni catalyst in in-situ hydrodeoxygenation of phenol....

Hydrogen recombiner catalyst test supporting data

International Nuclear Information System (INIS)

Britton, M.D.

1995-01-01

This is a data package supporting the Hydrogen Recombiner Catalyst Performance and Carbon Monoxide Sorption Capacity Test Report, WHC-SD-WM-TRP-211, Rev 0. This report contains 10 appendices which consist of the following: Mass spectrometer analysis reports: HRC samples 93-001 through 93-157; Gas spectrometry analysis reports: HRC samples 93-141 through 93-658; Mass spectrometer procedure PNL-MA-299 ALO-284; Alternate analytical method for ammonia and water vapor; Sample log sheets; Job Safety analysis; Certificate of mixture analysis for feed gases; Flow controller calibration check; Westinghouse Standards Laboratory report on Bois flow calibrator; and Sorption capacity test data, tables, and graphs

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

NARCIS (Netherlands)

Xie, Jingxiu; Torres Galvis, Hirsa; Koeken, Ard C J; Kirilin, Alexey; Dugulan, A Iulian; Ruitenbeek, Matthijs; de Jong, Krijn P

2016-01-01

The Fischer-Tropsch Synthesis converts synthesis gas from alternative carbon resources, including natural gas, coal, and biomass, to hydrocarbons used as fuels or chemicals. In particular, iron-based catalysts at elevated temperatures favor the selective production of C2-C4 olefins, which are

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.

Catalytic Transfer Hydrogenation of Furfural to Furfuryl Alcohol over Nitrogen-Doped Carbon-Supported Iron Catalysts.

Science.gov (United States)

Li, Jiang; Liu, Jun-Ling; Zhou, Hong-Jun; Fu, Yao

2016-06-08

Iron-based heterogeneous catalysts, which were generally prepared by pyrolysis of iron complexes on supports at elevated temperature, were found to be capable of catalyzing the transfer hydrogenation of furfural (FF) to furfuryl alcohol (FFA). The effects of metal precursor, nitrogen precursor, pyrolysis temperature, and support on catalytic performance were examined thoroughly, and a comprehensive study of the reaction parameters was also performed. The highest selectivity of FFA reached 83.0 % with a FF conversion of 91.6 % under the optimal reaction condition. Catalyst characterization suggested that iron cations coordinated by pyridinic nitrogen functionalities were responsible for the enhanced catalytic activity. The iron catalyst could be recycled without significant loss of catalytic activity for five runs, and the destruction of the nitrogen-iron species, the presence of crystallized Fe2 O3 phase, and the pore structure change were the main reasons for catalyst deactivation. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Supported catalyst systems and method of making biodiesel products using such catalysts

Science.gov (United States)

Kim, Manhoe; Yan, Shuli; Salley, Steven O.; Ng, K. Y. Simon

2015-10-20

A heterogeneous catalyst system, a method of preparing the catalyst system and a method of forming a biodiesel product via transesterification reactions using the catalyst system is disclosed. The catalyst system according to one aspect of the present disclosure represents a class of supported mixed metal oxides that include at least calcium oxide and another metal oxide deposited on a lanthanum oxide or cerium oxide support. Preferably, the catalysts include CaO--CeO.sub.2ZLa.sub.2O.sub.3 or CaO--La.sub.2O.sub.3/CeO.sub.2. Optionally, the catalyst may further include additional metal oxides, such as CaO--La.sub.2O.sub.3--GdOxZLa.sub.2O.sub.3.

Co-Assembled Supported Catalysts: Synthesis of Nano-Structured Supported Catalysts with Hierarchic Pores through Combined Flow and Radiation Induced Co-Assembled Nano-Reactors

Directory of Open Access Journals (Sweden)

Galip Akay

2016-05-01

Full Text Available A novel generic method of silica supported catalyst system generation from a fluid state is presented. The technique is based on the combined flow and radiation (such as microwave, thermal or UV induced co-assembly of the support and catalyst precursors forming nano-reactors, followed by catalyst precursor decomposition. The transformation from the precursor to supported catalyst oxide state can be controlled from a few seconds to several minutes. The resulting nano-structured micro-porous silica supported catalyst system has a surface area approaching 300 m2/g and X-ray Diffraction (XRD-based catalyst size controlled in the range of 1–10 nm in which the catalyst structure appears as lamellar sheets sandwiched between the catalyst support. These catalyst characteristics are dependent primarily on the processing history as well as the catalyst (Fe, Co and Ni studied when the catalyst/support molar ratio is typically 0.1–2. In addition, Ca, Mn and Cu were used as co-catalysts with Fe and Co in the evaluation of the mechanism of catalyst generation. Based on extensive XRD, Scanning Electron Microscopy (SEM and Transmission Electron Microscopy (TEM studies, the micro- and nano-structure of the catalyst system were evaluated. It was found that the catalyst and silica support form extensive 0.6–2 nm thick lamellar sheets of 10–100 nm planar dimensions. In these lamellae, the alternate silica support and catalyst layer appear in the form of a bar-code structure. When these lamellae structures pack, they form the walls of a micro-porous catalyst system which typically has a density of 0.2 g/cm3. A tentative mechanism of catalyst nano-structure formation is provided based on the rheology and fluid mechanics of the catalyst/support precursor fluid as well as co-assembly nano-reactor formation during processing. In order to achieve these structures and characteristics, catalyst support must be in the form of silane coated silica nano

Synthesis of 2-Substituted Benzofurans from o-Iodophenols and Terminal Alkynes with a Recyclable Palladium Catalyst Supported on Nano-sized Carbon Balls under Copper- and Ligand-Free Conditions

Energy Technology Data Exchange (ETDEWEB)

Yum, Eul Kgun; Yang, Okkyung; Kim, Jieun; Park, Hee Jank [Chungnam National Univ., Daejeon (Korea, Republic of)

2013-09-15

We have developed a one-step synthesis of benzofurans from o-iodophenol and various terminal alkynes, by using Pd catalyst supported on nano-sized carbon balls (NCB) under copper- and ligand free conditions. This recyclable catalyst could be reused more than 5 times in the same heteroannulation reaction. The results have demonstrated that diverse 2-substituted benzofurans with tolerant functional groups can be prepared simply and conveniently under these conditions.

Synthesis of 2-Substituted Benzofurans from o-Iodophenols and Terminal Alkynes with a Recyclable Palladium Catalyst Supported on Nano-sized Carbon Balls under Copper- and Ligand-Free Conditions

International Nuclear Information System (INIS)

Yum, Eul Kgun; Yang, Okkyung; Kim, Jieun; Park, Hee Jank

2013-01-01

We have developed a one-step synthesis of benzofurans from o-iodophenol and various terminal alkynes, by using Pd catalyst supported on nano-sized carbon balls (NCB) under copper- and ligand free conditions. This recyclable catalyst could be reused more than 5 times in the same heteroannulation reaction. The results have demonstrated that diverse 2-substituted benzofurans with tolerant functional groups can be prepared simply and conveniently under these conditions

Carbon supported ultrafine gold phosphorus nanoparticles as highly efficient electrocatalyst for alkaline ethanol oxidation reaction

International Nuclear Information System (INIS)

Li, Tongfei; Fu, Gengtao; Su, Jiahui; Wang, Yi; Lv, Yinjie; Zou, Xiuyong; Zhu, Xiaoshu; Xu, Lin; Sun, Dongmei; Tang, Yawen

2017-01-01

Graphical abstract: We develop a new kind of carbon supported gold-phosphorus (Au-P/C) electrocatalyst by a facile and novel phosphorus reduction method, and demonstrate the Au-P/C is a highly active and stable electrocatalyst for the ethanol oxidation reaction. - Highlights: • Au-P/C catalyst is synthesized by a facile and novel white-phosphorus reduce method. • AuP particles with ultrafine particle-size are uniformly dispersed on carbon support. • Au-P/C catalyst exhibits much higher content of P 0 than reported metal/P catalysts. • Au-P/C catalysts show excellent catalytic properties for ethanol oxidation reaction. - Abstract: Herein, we develop a new kind of carbon supported gold-phosphorus (Au-P/C) electrocatalyst for the alkaline ethanol oxidation reaction (EOR). The Au-P/C catalysts with different Au/P ratio (i.e., AuP/C, Au 3 P 2 /C and Au 4 P 3 /C) can be obtained by a facile and novel hot-reflux method with white phosphorus (P 4 ) as reductant and ethanol as solvent. The crystal structure, composition and particle-size of the Au-P/C catalysts are investigated by X-ray diffraction (XRD), Energy Dispersive Spectrometer (EDS), scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS), etc. The results demonstrate that Au-P/C catalysts present an alloy phase with the high content of P, ultrafine particle-size and high dispersity on carbon support, which results in excellent electrocatalytic activity and stability towards the EOR compared with that of the free-phosphorus Au/C catalyst. In addition, among the various Au-P/C catalysts with different Au/P ratio, the AuP/C sample exhibits the best electrocatalytic performance in comparison with other Au 3 P 2 /C and Au 4 P 3 /C samples.

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.

Attrition resistant Fischer-Tropsch catalyst and support

Science.gov (United States)

Singleton, Alan H.; Oukaci, Rachid; Goodwin, James G.

2004-05-25

A catalyst support having improved attrition resistance and a catalyst produced therefrom. The catalyst support is produced by a method comprising the step of treating calcined .gamma.-alumina having no catalytic material added thereto with an acidic aqueous solution having an acidity level effective for increasing the attrition resistance of the calcined .gamma.-alumina.

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.

N-Doped Carbon Xerogels as Pt Support for the Electro-Reduction of Oxygen

Directory of Open Access Journals (Sweden)

Cinthia Alegre

2017-09-01

Full Text Available Durability and limited catalytic activity are key impediments to the commercialization of polymer electrolyte fuel cells. Carbon materials employed as catalyst support can be doped with different heteroatoms, like nitrogen, to improve both catalytic activity and durability. Carbon xerogels are nanoporous carbons that can be easily synthesized in order to obtain N-doped materials. In the present work, we introduced melamine as a carbon xerogel precursor together with resorcinol for an effective in-situ N doping (3–4 wt % N. Pt nanoparticles were supported on nitrogen-doped carbon xerogels and their activity for the oxygen reduction reaction (ORR was evaluated in acid media along with their stability. Results provide new evidences of the type of N groups aiding the activity of Pt for the ORR and of a remarkable stability for N-doped carbon-supported Pt catalysts, providing appropriate physico-chemical features.

Hydrogen production by steam reforming of liquefied natural gas (LNG) over nickel catalysts supported on cationic surfactant-templated mesoporous aluminas

Science.gov (United States)

Seo, Jeong Gil; Youn, Min Hye; Park, Sunyoung; Jung, Ji Chul; Kim, Pil; Chung, Jin Suk; Song, In Kyu

Two types of mesoporous γ-aluminas (denoted as A-A and A-S) are prepared by a hydrothermal method under different basic conditions using cationic surfactant (cetyltrimethylammonium bromide, CTAB) as a templating agent. A-A and A-S are synthesized in a medium of ammonia solution and sodium hydroxide solution, respectively. Ni/γ-Al 2O 3 catalysts (Ni/A-A and Ni/A-S) are then prepared by an impregnation method, and are applied to hydrogen production by steam reforming of liquefied natural gas (LNG). The effect of a mesoporous γ-Al 2O 3 support on the catalytic performance of Ni/γ-Al 2O 3 is investigated. The identity of basic solution strongly affects the physical properties of the A-A and A-S supports. The high surface-area of the mesoporous γ-aluminas and the strong metal-support interaction of supported catalysts greatly enhance the dispersion of nickel species on the catalyst surface. The well-developed mesopores of the Ni/A-A and Ni/A-S catalysts prohibit the polymerization of carbon species on the catalyst surface during the reaction. In the steam reforming of LNG, both Ni/A-A and Ni/A-S catalysts give better catalytic performance than the nickel catalyst supported on commercial γ-Al 2O 3 (Ni/A-C). In addition, the Ni/A-A catalyst is superior to the Ni/A-S catalyst. The relatively strong metal-support interaction of Ni/A-A catalyst effectively suppresses the sintering of metallic nickel and the carbon deposition in the steam reforming of LNG. The large pores of the Ni/A-A catalyst also play an important role in enhancing internal mass transfer during the reaction.

Isotopic exchange between deuterium and neohexane on supported platinum and palladium catalysts

International Nuclear Information System (INIS)

Eskinazi, V.

1979-01-01

The isotopic exchange reaction between neohexane and deuterium on supported Pt/SiO 2 and Pd/SiO 2 catalysts has been investigated in the temperature range 86.5 to 110 0 C. Rates of exchange were studied as functions of percentage of metal atoms exposed, the conditions of catalyst pretreatment, and the reaction temperature. The rates of exchange were not strongly dependent upon percentage exposed; however, the relative yields of d 1 through d 5 in the ethyl moiety or neohexane were dependent on the percentage metal atoms exposed. The Pt/SiO 2 catalysts were found to be more active for exchange than the Pd/SiO 2 catalysts by an order of magnitude. Both the turnover frequencies and the exchange pattern were observed to be influenced by the pretreatment of the catalyst. Maxima in the exchange pattern occurred at d 3 and d 5 in the case of Pt/SiO 2 and at d 5 only in the case of the Pd/SiO 2 catalysts. In order to account for the d 3 maximum observed for Pt catalysts, some extension of the Horiuti-Polanyi mechanism is required. Mechanisms by which the d 3 species might be formed are proposed and discussed. On Pd/SiO 2 catalysts exchange occurs preferentially in the ethyl substituent of the quaternary carbon atom rather than on the three methyl substituents of the quaternary carbon atom. Such preference is not observed on Pt/SiO 2 catalysts; in fact, in some cases, this preference is reversed. Whenever exchange occurs in the three methyl substituents, mostly the d 1 product is obtained. For Pt/SiO 2 catalysts, the exchange pattern appears to be influenced by steric effects, but the data suggest that factors other than steric effects are important on Pd

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

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...

Fundamental Studies of the Reforming of Oxygenated Compounds over Supported Metal Catalysts

Energy Technology Data Exchange (ETDEWEB)

Dumesic, James A. [Univ. of Wisconsin, Madison, WI (United States)

2016-01-04

The main objective of our research has been to elucidate fundamental concepts associated with controlling the activity, selectivity, and stability of bifunctional, metal-based heterogeneous catalysts for tandem reactions, such as liquid-phase conversion of oxygenated hydrocarbons derived from biomass. We have shown that bimetallic catalysts that combine a highly-reducible metal (e.g., platinum) with an oxygen-containing metal promoter (e.g., molybdenum) are promising materials for conversion of oxygenated hydrocarbons because of their high activity for selective cleavage for carbon-oxygen bonds. We have developed methods to stabilize metal nanoparticles against leaching and sintering under liquid-phase reaction conditions by using atomic layer deposition (ALD) to apply oxide overcoat layers. We have used controlled surface reactions to produce bimetallic catalysts with controlled particle size and controlled composition, with an important application being the selective conversion of biomass-derived molecules. The synthesis of catalysts by traditional methods may produce a wide distribution of metal particle sizes and compositions; and thus, results from spectroscopic and reactions kinetics measurements have contributions from a distribution of active sites, making it difficult to assess how the size and composition of the metal particles affect the nature of the surface, the active sites, and the catalytic behavior. Thus, we have developed methods to synthesize bimetallic nanoparticles with controlled particle size and controlled composition to achieve an effective link between characterization and reactivity, and between theory and experiment. We have also used ALD to modify supported metal catalysts by addition of promoters with atomic-level precision, to produce new bifunctional sites for selective catalytic transformations. We have used a variety of techniques to characterize the metal nanoparticles in our catalysts, including scanning transmission electron

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)

Supported phosphate and carbonate salts for heterogeneous catalysis of triglycerides to fatty acid methyl esters

Science.gov (United States)

Britton, Stephanie Lynne

Fatty acid methyl esters made from vegetable oil, or biodiesel, have been identified as a substitute for diesel derived from crude oil. Biodiesel is currently made using a homogeneous base catalyst to perform the transesterification of triglycerides with methanol to generate fatty acid methyl esters (FAME). The use of a homogeneous catalyst necessitates additional purification of the product and byproducts before sale, and the catalyst is consumed and discarded. The development of a heterogeneous basic catalyst for the production of FAME is desirable. Tribasic phosphate salts and dibasic carbonate salts are active for the production of FAME but generally operate as homogeneous catalysts. Supporting these phosphate and carbonate salts on mesoporous MCM-41, microporous silica gel, and nonporous a-alumina proved successful to greater or lesser degrees depending on the identity of the support and pretreatment of the support. Although these salts were supported and were active for the production of FAME from canola oil, they proved to be operating as homogeneous catalysts due to leaching of the active species off the surface of the support. Further investigation of the active species present in the tribasic phosphate catalysts identified the active support as orthophosphate, and NMR studies revealed the phosphorus to be present as orthophosphate and diphosphate in varying proportions in each catalyst. Evaluation of the acid-washing support pretreatment process revealed that the exposure of the support to acid plays a large role in the development of activity on the surface of the catalyst, but manipulation of these parameters did not prevent leaching of the active site off the surface of the catalyst. Alternate methods of support pretreatment were no more effective in preventing leaching. Tribasic phosphate supported on silica gel is not effective as a heterogeneous catalyst for FAME production from triglycerides because of the lack of stability of the phosphate on the

Graphite-supported platinum catalysts: Effects of gas and aqueous phase treatments

Energy Technology Data Exchange (ETDEWEB)

Vleeming, J.H.; Kuster, B.F.M.; Marin, G.B. [Eindhoven Univ. of Technology (Netherlands)] [and others

1997-03-01

The effects on the platinum particle diameter and the available platinum surface area of a graphite-supported platinum catalyst resulting from pretreatments and from performing a selective oxidation reaction are investigated. In the gas phase considerable catalyst sintering occurs only in the presence of oxygen at 773 K due to extensive carbon burn-off, whereas in an aqueous phase platinum particle growth is limited upon oxidative treatment. A hydrogen treatment in aqueous phase at 363 K causes platinum particle growth, aggregate formation, and covering of metal sites. These phenomena become more important with increasing pH. Platinum particle growth and aggregate formation are attributed to platinum particle rather than platinum adatom mobility and is caused by the destruction of the oxygen-containing surface groups on the graphite support, which serve as anchorage sites for the platinum particles. Site covering is caused by products originating from the graphite support, which are formed as a result of the reductive treatments. When performing the aqueous phase oxidation of methyl {alpha}-D-glucopyranoside at 323 K and a pH of 9, catalyst modifications are small under oxidative conditions. Exposure of the catalyst for several hours to methyl {alpha}-D-glucopyranoside under the same conditions but in the absence of oxygen causes site covering. 50 refs., 9 figs., 1 tab.

Titanium Dioxide as a Catalyst Support in Heterogeneous Catalysis

Science.gov (United States)

Bagheri, Samira; Muhd Julkapli, Nurhidayatullaili; Bee Abd Hamid, Sharifah

2014-01-01

The lack of stability is a challenge for most heterogeneous catalysts. During operations, the agglomeration of particles may block the active sites of the catalyst, which is believed to contribute to its instability. Recently, titanium oxide (TiO2) was introduced as an alternative support material for heterogeneous catalyst due to the effect of its high surface area stabilizing the catalysts in its mesoporous structure. TiO2 supported metal catalysts have attracted interest due to TiO2 nanoparticles high activity for various reduction and oxidation reactions at low pressures and temperatures. Furthermore, TiO2 was found to be a good metal oxide catalyst support due to the strong metal support interaction, chemical stability, and acid-base property. The aforementioned properties make heterogeneous TiO2 supported catalysts show a high potential in photocatalyst-related applications, electrodes for wet solar cells, synthesis of fine chemicals, and others. This review focuses on TiO2 as a support material for heterogeneous catalysts and its potential applications. PMID:25383380

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.

N, P-codoped Mesoporous Carbon Supported PtCox Nanoparticles and Their Superior Electrochemical toward Methanol Oxidation

Science.gov (United States)

Cui, Hangjun; Li, Yueming; Liu, Shimin

2018-03-01

In this report, a novel strategy by using the N, P co-doped mesoporous carbon structure as catalyst support to enhance the electrochemical catalytic activity of Pt-based catalysts is proposed. The as-synthesized PtCox@N, P-doped mesoporous carbon nanocomposties have been studied as an anode catalyst toward methanol oxidation, exhibiting greatly improved electrochemical activity and stability compared with Pt@mesoporous carbon. The synergistic effects of N, P dual-doping and porous carbon structure help to achieve better electron transport at the electrode surface, which eventually leads to greatly enhanced catalytic activity compared to the pristine Pt/mesoporous carbon.…

Copolymerization of carbon monoxide and styrene catalyzed by resin-supported palladium polymer

Directory of Open Access Journals (Sweden)

2007-02-01

Full Text Available Polyketone was prepared by the copolymerization of carbon monoxide (CO and styrene (ST catalyzed by o-phenylenediamine resin-supported palladium acetate. Effects of each catalytic system component such as 2,2’-bipyridine, 1,4-quinone and p-toluene-sulphonate on the copolymerization were investigated. The resin-supported catalyst and the copolymerization product were characterized by infrared spectroscopy (IR, differential scanning calorimetry (DSC, thermogravimetry (TG, X-ray photoelectron spectroscopy (XPS, Scanning Electron Microscopy (SEM. Results indicated that the resin-supported catalyst has excellent catalytic property. Furthermore, partial catalytic activity was maintained after the catalyst was used for five times.

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.

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.

Steam Reforming of Acetic Acid over Co-Supported Catalysts: Coupling Ketonization for Greater Stability

Energy Technology Data Exchange (ETDEWEB)

Davidson, Stephen D. [Energy and Environmental; Spies, Kurt A. [Energy and Environmental; Mei, Donghai [Energy and Environmental; Kovarik, Libor [Energy and Environmental; Kutnyakov, Igor [Energy and Environmental; Li, Xiaohong S. [Energy and Environmental; Lebarbier Dagle, Vanessa [Energy and Environmental; Albrecht, Karl O. [Energy and Environmental; Dagle, Robert A. [Energy and Environmental

2017-09-11

We report on the markedly improved stability of a novel 2-bed catalytic system, as compared to a conventional 1-bed steam reforming catalyst, for the production of H2 from acetic acid. The 2-bed catalytic system comprises of i) a basic oxide ketonization catalyst for the conversion of acetic acid to acetone, and a ii) Co-based steam reforming catalyst, both catalytic beds placed in sequence within the same unit operation. Steam reforming catalysts are particularly prone to catalytic deactivation when steam reforming acetic acid, used here as a model compound for the aqueous fraction of bio-oil. Catalysts comprising MgAl2O4, ZnO, CeO2, and activated carbon (AC) both with and without Co-addition were evaluated for conversion of acetic acid and acetone, its ketonization product, in the presence of steam. It was found that over the bare oxide support only ketonization activity was observed and coke deposition was minimal. With addition of Co to the oxide support steam reforming activity was facilitated and coke deposition was significantly increased. Acetone steam reforming over the same Co-supported catalysts demonstrated more stable performance and with less coke deposition than with acetic acid feedstock. DFT analysis suggests that over Co surface CHxCOO species are more favorably formed from acetic acid versus acetone. These CHxCOO species are strongly bound to the Co catalyst surface and could explain the higher propensity for coke formation from acetic acid. Based on these findings, in order to enhance stability of the steam reforming catalyst a dual-bed (2-bed) catalyst system was implemented. Comparing the 2-bed and 1-bed (Co-supported catalyst only) systems under otherwise identical reaction conditions the 2-bed demonstrated significantly improved stability and coke deposition was decreased by a factor of 4.

Spatially and size selective synthesis of Fe-based nanoparticles on ordered mesoporous supports as highly active and stable catalysts for ammonia decomposition.

Science.gov (United States)

Lu, An-Hui; Nitz, Joerg-Joachim; Comotti, Massimiliano; Weidenthaler, Claudia; Schlichte, Klaus; Lehmann, Christian W; Terasaki, Osamu; Schüth, Ferdi

2010-10-13

Uniform and highly dispersed γ-Fe(2)O(3) nanoparticles with a diameter of ∼6 nm supported on CMK-5 carbons and C/SBA-15 composites were prepared via simple impregnation and thermal treatment. The nanostructures of these materials were characterized by XRD, Mössbauer spectroscopy, XPS, SEM, TEM, and nitrogen sorption. Due to the confinement effect of the mesoporous ordered matrices, γ-Fe(2)O(3) nanoparticles were fully immobilized within the channels of the supports. Even at high Fe-loadings (up to about 12 wt %) on CMK-5 carbon no iron species were detected on the external surface of the carbon support by XPS analysis and electron microscopy. Fe(2)O(3)/CMK-5 showed the highest ammonia decomposition activity of all previously described Fe-based catalysts in this reaction. Complete ammonia decomposition was achieved at 700 °C and space velocities as high as 60,000 cm(3) g(cat)(-1) h(-1). At a space velocity of 7500 cm(3) g(cat)(-1) h(-1), complete ammonia conversion was maintained at 600 °C for 20 h. After the reaction, the immobilized γ-Fe(2)O(3) nanoparticles were found to be converted to much smaller nanoparticles (γ-Fe(2)O(3) and a small fraction of nitride), which were still embedded within the carbon matrix. The Fe(2)O(3)/CMK-5 catalyst is much more active than the benchmark NiO/Al(2)O(3) catalyst at high space velocity, due to its highly developed mesoporosity. γ-Fe(2)O(3) nanoparticles supported on carbon-silica composites are structurally much more stable over extended periods of time but less active than those supported on carbon. TEM observation reveals that iron-based nanoparticles penetrate through the carbon layer and then are anchored on the silica walls, thus preventing them from moving and sintering. In this way, the stability of the carbon-silica catalyst is improved. Comparison with the silica supported iron oxide catalyst reveals that the presence of a thin layer of carbon is essential for increased catalytic activity.

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.

Immobilization of molecular catalysts in supported ionic liquid phases.

Science.gov (United States)

Van Doorslaer, Charlie; Wahlen, Joos; Mertens, Pascal; Binnemans, Koen; De Vos, Dirk

2010-09-28

In a supported ionic liquid phase (SILP) catalyst system, an ionic liquid (IL) film is immobilized on a high-surface area porous solid and a homogeneous catalyst is dissolved in this supported IL layer, thereby combining the attractive features of homogeneous catalysts with the benefits of heterogeneous catalysts. In this review reliable strategies for the immobilization of molecular catalysts in SILPs are surveyed. In the first part, general aspects concerning the application of SILP catalysts are presented, focusing on the type of catalyst, support, ionic liquid and reaction conditions. Secondly, organic reactions in which SILP technology is applied to improve the performance of homogeneous transition-metal catalysts are presented: hydroformylation, metathesis reactions, carbonylation, hydrogenation, hydroamination, coupling reactions and asymmetric reactions.

Mesoporous TiO2 : an alternative material for PEM fuel cells catalyst support

Energy Technology Data Exchange (ETDEWEB)

Do, T.B. [Michigan Univ., Ann Arbor, MI (United States). Dept. of Materials Science; Ruthkosky, M.; Cai, M. [General Motors, Warren, MI (United States). Research and Development Center

2008-07-01

This paper discussed the feasibility of using an alternative catalyst support material to replace carbon in proton exchange membrane (PEM) fuel cells. The alternative catalyst support material requires a high surface area with a large porosity but must have comparable conductivity with carbon. A mesoporous titanium oxide (TiO2) material produced by coprecipitation was introduced. The conductivity of the material is about one order of that of carbon. The 8 mole per cent Nb-doped TiO2 was formed and deposited on the surface of a nano polystyrene (PS) template via the hydrolysis of a co-solution of Ti(OC4H9)4 and Nb(OC2H5)5. The removal of PS by heat treatment produced porous structure of TiO2 with the appearance of 3 different pore types, notably open pore, ink-pot pores and closed pores. TiO2 formed from the rutile phase, allowing a lower activation temperature at 850 degrees C in a hydrogen atmosphere. The pore structures were retained after this heat treatment. The BET surface area was 116 m{sup 2}/g, porosity was 22 per cent and the average pore size was 159 angstrom. The conductivity improved considerably from almost non-conductive to one order of that of carbon.

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.

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.

Thermal decomposition of supported lithium nitrate catalysts

Energy Technology Data Exchange (ETDEWEB)

Ruiz, Maria Lucia [INTEQUI (CONICET-UNSL), 25 de Mayo 384, V. Mercedes, 5730, San Luis (Argentina); Lick, Ileana Daniela [CINDECA (CONICET-UNLP), Calle 47 No 257, La Plata, 1900, Buenos Aires (Argentina); Ponzi, Marta Isabel [INTEQUI (CONICET-UNSL), 25 de Mayo 384, V. Mercedes, 5730, San Luis (Argentina); Castellon, Enrique Rodriguez; Jimenez-Lopez, Antonio [Departamento de Quimica Inorganica, Cristalografia y Mineralogia. Facultad de Ciencias, Universidad de Malaga, Campus de Teatinos, 29071 Malaga (Spain); Ponzi, Esther Natalia, E-mail: eponzi@quimica.unlp.edu.ar [CINDECA (CONICET-UNLP), Calle 47 No 257, La Plata, 1900, Buenos Aires (Argentina)

2010-02-20

New catalysts for soot combustion were prepared by impregnation of different supports (SiO{sub 2}, ZrO{sub 2} and ZrO{sub 2}.nH{sub 2}O) with a LiNO{sub 3} solution and then characterized by means of FTIR, XPS, TGA and UV-vis spectroscopy, whereby the presence of lithium nitrate in the prepared catalysts was identified and quantified. The soot combustion rate using this series of catalysts (LiNO{sub 3}/support) was compared with the activity of a series of impregnated catalysts prepared using LiOH (Li{sub 2}O/supports). Catalysts prepared using LiNO{sub 3} are found to be more active than those prepared using LiOH. The catalytic performance was also studied with a NO/O{sub 2} mixture in the feed, demonstrating that NO increases the combustion rate of soot, probably as a consequence of lithium oxide forming an 'in situ' nitrate ion.

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

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.

Catalytic transformation of carbon dioxide and methane into syngas over ruthenium and platinum supported hydroxyapatites

International Nuclear Information System (INIS)

Rêgo De Vasconcelos, Bruna; Zhao, Lulu; Sharrock, Patrick; Nzihou, Ange; Pham Minh, Doan

2016-01-01

Highlights: • Formation of nanoparticles of Pt and Ru on hydroxyapatite surface support (HAP). • Pt catalyst more active and stable than Ru catalyst in dry reforming of methane (DRM). • Low carbon deposition on the surface of Pt catalyst after reaction. • Quantification of water as by-product of the reaction for the first time. • Good mass balance of the reaction. - Abstract: This work focused on the catalytic transformation of methane (CH 4 ) and carbon dioxide (CO 2 ) into syngas (mixture of CO and H 2 ). Ruthenium- and platinum-based catalysts were prepared using hydroxyapatite (HAP) as catalyst support. Different methods for metal deposition were used including incipient wetness impregnation (IWI), excess liquid phase impregnation (LIM), and cationic exchange (CEX). Metal particle size varied in large range from less than 1 nm to dozens nm. All catalysts were active at 400–700 °C but only Pt catalyst prepared by IWI method (Pt/HAP IWI) was found stable. The catalytic performance of Pt/HAP IWI could be comparable with the literature data on noble metal-based catalysts, prepared on metal oxide supports. For the first time, water was experimentally quantified as a by-product of the reaction. This helped to correctly buckle the mass balance of the process.

Catalytic transformation of carbon dioxide and methane into syngas over ruthenium and platinum supported hydroxyapatites

Energy Technology Data Exchange (ETDEWEB)

Rêgo De Vasconcelos, Bruna; Zhao, Lulu; Sharrock, Patrick; Nzihou, Ange; Pham Minh, Doan, E-mail: doan.phamminh@mines-albi.fr

2016-12-30

Highlights: • Formation of nanoparticles of Pt and Ru on hydroxyapatite surface support (HAP). • Pt catalyst more active and stable than Ru catalyst in dry reforming of methane (DRM). • Low carbon deposition on the surface of Pt catalyst after reaction. • Quantification of water as by-product of the reaction for the first time. • Good mass balance of the reaction. - Abstract: This work focused on the catalytic transformation of methane (CH{sub 4}) and carbon dioxide (CO{sub 2}) into syngas (mixture of CO and H{sub 2}). Ruthenium- and platinum-based catalysts were prepared using hydroxyapatite (HAP) as catalyst support. Different methods for metal deposition were used including incipient wetness impregnation (IWI), excess liquid phase impregnation (LIM), and cationic exchange (CEX). Metal particle size varied in large range from less than 1 nm to dozens nm. All catalysts were active at 400–700 °C but only Pt catalyst prepared by IWI method (Pt/HAP IWI) was found stable. The catalytic performance of Pt/HAP IWI could be comparable with the literature data on noble metal-based catalysts, prepared on metal oxide supports. For the first time, water was experimentally quantified as a by-product of the reaction. This helped to correctly buckle the mass balance of the process.

Nano-Scale Au Supported on Carbon Materials for the Low Temperature Water Gas Shift (WGS Reaction

Directory of Open Access Journals (Sweden)

Paula Sánchez

2011-12-01

Full Text Available Au-based catalysts supported on carbon materials with different structures such as graphite (G and fishbone type carbon nanofibers (CNF-F were prepared using two different methods (impregnation and gold-sol to be tested in the water gas shift (WGS reaction. Atomic absorption spectrometry, transmission electron microscopy (TEM, temperature-programmed oxidation (TPO, X-ray diffraction (XRD, Raman spectroscopy, elemental analyses (CNH, N2 adsorption-desorption analysis, temperature-programmed reduction (TPR and temperature-programmed decomposition were employed to characterize both the supports and catalysts. Both the crystalline nature of the carbon supports and the method of gold incorporation had a strong influence on the way in which Au particles were deposited on the carbon surface. The higher crystallinity and the smaller and well dispersed Au particle size were, the higher activity of the catalysts in the WGS reaction was noted. Finally, catalytic activity showed an important dependence on the reaction temperature and steam-to-CO molar ratio.

Adsorption and oxidation of acetaldehyde on carbon supported Pt, PtSn and PtSn-based trimetallic catalysts by in situ Fourier transform infrared spectroscopy

Science.gov (United States)

Beyhan, Seden; Léger, Jean-Michel; Kadırgan, Figen

2013-11-01

The adsorption and oxidation of acetaldehyde on carbon supported Pt, Pt90Sn10 and Pt80Sn10M10 (M = Ni, Co, Rh, Pd) catalysts have been investigated by using in situ Fourier transform infrared (FTIR) spectroscopy. The result revealed that Pt90Sn10/C catalyst is not very efficient for the conversion of acetaldehyde to CO2 due to the weak adsorption of acetaldehyde in the presence of Sn. However, the addition of a third metal to Pt--Sn facilitates the C-C bond cleavage of acetaldehyde. It seems that acetaldehyde is adsorbed dissociatively on the surface of Pt80Sn10Ni10/C, Pt80Sn10Co10/C, Pt80Sn10Rh10/C catalysts, producing CH3 and CHO adsorbate species, which can be further oxidized to CO2. However, the pathway forming CO2 for Pt80Sn10Pd10/C catalyst mainly originates from the oxidation of CH3CO species. Thus, the presence of third metal in the PtSn catalyst has a strong impact upon the acetaldehyde adsorption behaviour and its reaction products.

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)

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.

Catalytic oxidation of albendazole using molybdenum supported on carbon nanotubes as catalyst; Oxidacion catalitica de albendazol empleando como catalizador molibdeno soportado en nanotubos de carbono

Energy Technology Data Exchange (ETDEWEB)

Sun-Kou, Maria del Rosario; Vega Carrasco, Edgar R., E-mail: msun@pucp.edu.pe [Departamento de Ciencias, Seccion Quimica. Pontificia Universidad Catolica del Peru, Avenida Universitaria 1801, Lima (Peru); Picasso Escobar, Gino I. [Laboratorio de Investigacion de Fisicoquimica, Facultad de Ciencias, Universidad Nacional de Ingenieria, Avenida Tupac Amaru 210, Lima (Peru)

2013-10-15

The catalytic oxidation reaction of the thioether group (-S-) in the structure to the drug albendazole (C{sub 12}H{sub 15}N{sub 3}O{sub 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 {sup o}C. For the catalytic oxidation reaction was employed hydrogen peroxide-urea (H{sub 2}NCONH{sub 2}·H{sub 2}O{sub 2}) as oxidizing agent and methanol (CH{sub 3}OH) as reaction medium. The textural and morphology characterization of carbon nanoparticles and catalysts was carried out by adsorption-desorption of N{sub 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)

Catalyst support structure, catalyst including the structure, reactor including a catalyst, and methods of forming same

Science.gov (United States)

Van Norman, Staci A.; Aston, Victoria J.; Weimer, Alan W.

2017-05-09

Structures, catalysts, and reactors suitable for use for a variety of applications, including gas-to-liquid and coal-to-liquid processes and methods of forming the structures, catalysts, and reactors are disclosed. The catalyst material can be deposited onto an inner wall of a microtubular reactor and/or onto porous tungsten support structures using atomic layer deposition techniques.

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

NiMo-sulfide supported on activated carbon to produce renewable diesel

Directory of Open Access Journals (Sweden)

Nancy Y Acelas

2017-03-01

Full Text Available Due to their weak polarity and large surface area, activated carbon supports have the potential to enhance the dispersion of metal-sulfides. It is expected that the absence of a strong metal-support interaction can result in the formation of a very active and stable Ni-Mo-S phase. In this study, catalysts with different amounts of nickel and molybdenum supported on a commercial activated carbon were prepared by a co-impregnation method and characterized by BET, XRF, and SEM techniques. The catalytic activity for hydroprocessing of Jatropha oil was evaluated in a batch reactor, and the composition of the liquid and gaseous products were determined. Results showed that gaseous products are mainly composed of high amounts of propane and small amounts of other light hydrocarbons (C1 to C5. Liquid hydrocarbon products consisted of a mixture containing mainly n-paraffins of C15-C18 and some oxygenated compounds. The catalysts with a mass fraction of 3 % Ni, 15 % Mo (Ni3Mo15/AC presented the highest selectivity toward C17-C18 hydrocarbons, with a product distribution similar to a commercial alumina-supported Ni-Mo-S catalyst.

Preparation of SnO{sub 2}-CNTs supported Pt catalysts and their electrocatalytic properties for ethanol oxidation

Energy Technology Data Exchange (ETDEWEB)

Pang, H.L.; Lu, J.P. [State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082 (China); Chen, J.H. [State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082 (China)], E-mail: chenjinhua@hnu.cn; Huang, C.T.; Liu, B.; Zhang, X.H. [State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082 (China)

2009-03-30

SnO{sub 2}-carbon nanotubes (CNTs) composites were prepared by sol-gel method, and characterized by scanning electron microscopy and X-ray diffraction. Due to high stability in diluted acidic solution, SnO{sub 2}-CNTs composites were selected as the catalyst support and second catalyst for ethanol electrooxidation. The electrocatalytic properties of the SnO{sub 2}-CNTs supported platinum (Pt) catalyst (Pt/SnO{sub 2}-CNTs) for ethanol oxidation have been investigated by typical electrochemical methods. Under the same mass loading of Pt, the Pt/SnO{sub 2}-CNTs catalyst shows higher electrocatalytic activity and better long-term cycle stability than Pt/SnO{sub 2} catalyst. Additionally, the effect of the mass ratio of CNTs to SnO{sub 2} on the electrocatalytic activity of the electrode for ethanol oxidation was investigated, and the optimum mass ratio of CNTs to SnO{sub 2} in the Pt/SnO{sub 2}-CNTs catalyst is 1/6.3.

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.)

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.

Predicting catalyst-support interactions between metal nanoparticles and amorphous silica supports

Science.gov (United States)

Ewing, Christopher S.; Veser, Götz; McCarthy, Joseph J.; Lambrecht, Daniel S.; Johnson, J. Karl

2016-10-01

Metal-support interactions significantly affect the stability and activity of supported catalytic nanoparticles (NPs), yet there is no simple and reliable method for estimating NP-support interactions, especially for amorphous supports. We present an approach for rapid prediction of catalyst-support interactions between Pt NPs and amorphous silica supports for NPs of various sizes and shapes. We use density functional theory calculations of 13 atom Pt clusters on model amorphous silica supports to determine linear correlations relating catalyst properties to NP-support interactions. We show that these correlations can be combined with fast discrete element method simulations to predict adhesion energy and NP net charge for NPs of larger sizes and different shapes. Furthermore, we demonstrate that this approach can be successfully transferred to Pd, Au, Ni, and Fe NPs. This approach can be used to quickly screen stability and net charge transfer and leads to a better fundamental understanding of catalyst-support interactions.

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.

Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane.

Science.gov (United States)

Zhang, Sheng; Kang, Peng; Bakir, Mohammed; Lapides, Alexander M; Dares, Christopher J; Meyer, Thomas J

2015-12-29

Developing sustainable energy strategies based on CO2 reduction is an increasingly important issue given the world's continued reliance on hydrocarbon fuels and the rise in CO2 concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO2 reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO2 reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO2 reduction to methane. The origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd-H sites and Cu-CO sites during electrochemical CO2 reduction. The polymer substrate also appears to provide a basis for the local concentration of CO2 resulting in the enhancement of catalytic current densities by threefold. The procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices.

Designing Pd-based supported bimetallic catalysts for environmental applications

OpenAIRE

Nowicka, Ewa; Meenakshisundaram, Sankar

2018-01-01

Supported bimetallic nanoparticulate catalysts are an important class of heterogeneous catalysts for many reactions including selective oxidation, hydrogenation/hydrogenolysis, reforming, biomass conversion reactions, and many more. The activity, selectivity, and stability of these catalysts depend on their structural features including particle size, composition, and morphology. In this review, we present important structural features relevant to supported bimetallic catalysts focusing on Pd...

Adhered Supported Carbon Nanotubes

International Nuclear Information System (INIS)

Johnson, Dale F.; Craft, Benjamin J.; Jaffe, Stephen M.

2001-01-01

Carbon nanotubes (NTs) in excess of 200 μm long are grown by catalytic pyrolysis of hydrocarbon vapors. The nanotubes grow continuously without the typical extinction due to catalyst encapsulation. A woven metal mesh supports the nanotubes creating a metal supported nanotube (MSNT) structure. The 140 μm wide mesh openings are completely filled by 70 nm diameter multiwalled nanotubes (MWNTs). The MWNTs are straight, uniform and highly crystalline. Their wall thickness is about 10 nm (30 graphite layers). The adherent NTs are not removed from the support in a Scotch tape pull test. A 12.5 cm 2 capacitor made from two MSNT structures immersed in 1 M KCl has a capacitance of 0.35 F and an equivalent series resistance of 0.18 Ω. Water flows through the MSNT at a flow velocity of 1 cm/min with a pressure drop of 15 inches of water. With the support removed, the MWNTs naturally form a carbon nanocomposite (CNC) paper with a specific area of 80 m 2 /gm, a bulk density of 0.21 g/cm 3 , an open pore fraction of 0.81, and a resistivity of 0.16 Ω-cm

Study of Supported Nickel Catalysts Prepared by Aqueous Hydrazine Method. Hydrogenating Properties and Hydrogen Storage: Support Effect. Silver Additive Effect; Catalyseurs de nickel supportes prepares par la methode de l'hydrazine aqueuse. Proprietes hydrogenantes et stockage d'hydrogene. Effet du support. Effet de l'ajout d'argent

Energy Technology Data Exchange (ETDEWEB)

Wojcieszak, R

2006-06-15

We have studied Ni or NiAg nano-particles obtained by the reduction of nickel salts (acetate or nitrate) by hydrazine and deposited by simple or EDTA-double impregnation on various supports ({gamma}-Al{sub 2}O{sub 3}, amorphous or crystallized SiO{sub 2}, Nb{sub 2}O{sub 5}, CeO{sub 2} and carbon). Prepared catalysts were characterized by different methods (XRD, XPS, low temperature adsorption and desorption of N{sub 2}, FTIR and FTIR-Pyridine, TEM, STEM, EDS, H{sub 2}-TPR, H{sub 2}-adsorption, H{sub 2}-TPD, isopropanol decomposition) and tested in the gas phase hydrogenation of benzene or as carbon materials in the hydrogen storage at room temperature and high pressure. The catalysts prepared exhibited better dispersion and activity than classical catalysts. TOF's of NiAg/SiO{sub 2} or Ni/carbon catalysts were similar to Pt catalysts in benzene hydrogenation. Differences in support acidity or preparation method and presence of Ag as metal additive play a crucial role in the chemical reduction of Ni by hydrazine and in the final properties of the materials. Ni/carbon catalysts could store significant amounts of hydrogen at room temperature and high pressure (0.53%/30 bars), probably through the hydrogen spillover effect. (author)

Catalyst systems and uses thereof

Science.gov (United States)

Ozkan, Umit S [Worthington, OH; Holmgreen, Erik M [Columbus, OH; Yung, Matthew M [Columbus, OH

2012-07-24

A method of carbon monoxide (CO) removal comprises providing an oxidation catalyst comprising cobalt supported on an inorganic oxide. The method further comprises feeding a gaseous stream comprising CO, and oxygen (O.sub.2) to the catalyst system, and removing CO from the gaseous stream by oxidizing the CO to carbon dioxide (CO.sub.2) in the presence of the oxidation catalyst at a temperature between about 20 to about 200.degree. C.

Multi-wall carbon nanotubes supported molybdenyl acetylacetonate: Efficient and highly reusable catalysts for epoxidation of alkenes with tert-butyl hydroperoxide

International Nuclear Information System (INIS)

Esnaashari, Fariba; Moghadam, Majid; Mirkhani, Valiollah; Tangestaninejad, Shahram; Mohammadpoor-Baltork, Iraj; Khosropour, Ahmad Reza; Zakeri, Maryam

2012-01-01

Efficient epoxidation of olefins catalyzed by MoO 2 (acac) 2 supported on amines functionalized MWCNTs is reported. The MWCNTs bearing carboxylic acid groups were modified with 2-aminophenol and 2-aminothiophenol. These amine–MWCNTs act as bidentate ligand for attachment of Mo catalyst. These catalysts were characterized by elemental analysis, scanning electron microscopy, FT-IR and diffuse reflectance UV–Vis spectroscopic methods. The prepared catalysts were used for efficient epoxidation of different alkenes such as cyclic and linear ones with tert-butyl hydroperoxide in refluxing 1,2-dichloroethane. These heterogeneous catalysts can be reused several times without significant loss of their catalytic activity. Highlights: ► Supporting of molybdenyl acetylacetonate on amine-modified MWCNTs. ► Heterogeneous catalysts were prepared. ► These catalysts were highly efficient in the epoxidation of alkenes with TBHP. ► Makes the catalysts reusable.

Microwave heated polyol synthesis of carbon supported PtAuSn/C nanoparticles for ethanol electrooxidation

Energy Technology Data Exchange (ETDEWEB)

Zhu, Hong; Han, Kefei [School of Science, State key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China); Liu, Yingli; Chang, Zhaorong [College of Chemistry and Environmental Science, Henan Normal University, Xinxiang, Henan (China); Shen, Liangbo [Beijing No.4 High School, Beijing (China); Wei, Yongsheng; Guo, Zhijun (School of Science Beijing Jiaotong University Beijing P. R. China); Wang, Haijiang [Institute for Fuel Cell Innovation, National Research Council of (Canada)

2010-04-15

Carbon-supported PtAuSn/C nanoparticle catalyst was synthesized by a microwave-assisted polyol process. The process is a quick process that only requires a few minutes to complete. The catalyst thus obtained was characterized by transmission electron microscopy and X-ray diffraction analysis. The electrochemical performance of the catalyst, for the ethanol oxidation reaction, was also investigated. The results indicated that the PtAuSn/C catalyst was uniformly dispersed on carbon and was in the nano-size range. The electrochemical measurements indicated that PtAuSn/C nanoparticle catalyst synthesized by the microwave-assisted polyol method demonstrated a significantly higher electrochemically active area and higher catalytic activity than Pt/C for the ethanol oxidation reaction. (author)

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 ...

Enhanced hydrogen reaction kinetics of nanostructured Mg-based composites with nanoparticle metal catalysts dispersed on supports

International Nuclear Information System (INIS)

Yoo, Yeong; Tuck, Mark; Kondakindi, Rajender; Seo, Chan-Yeol; Dehouche, Zahir; Belkacemi, Khaled

2007-01-01

Hydrogen reaction kinetics of nanocrystalline MgH 2 co-catalyzed with Ba 3 (Ca 1+x Nb 2-x )O 9-δ (BCN) proton conductive ceramics and nanoparticle bimetallic catalyst of Ni/Pd dispersed on single wall carbon nanotubes (SWNTs) support has been investigated. The nanoparticle bimetallic catalysts of Ni/Pd supported by SWNTs were synthesized based on a novel polyol method using NiCl 2 .6H 2 O, PdCl 2 , NaOH and ethylene glycol (EG). The nanostructured Mg composites co-catalyzed with BCN and bimetallic supported catalysts exhibited stable hydrogen desorption capacity of 6.3-6.7 wt.% H 2 and the significant enhancement of hydrogen desorption kinetics at 230-300 deg. C in comparison to either non-catalyzed MgH 2 or the nanocomposite of MgH 2 catalyzed with BCN

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.

Carbon nanotube-supported Au-Pd alloy with cooperative effect of metal nanoparticles and organic ketone/quinone groups as a highly efficient catalyst for aerobic oxidation of amines.

Science.gov (United States)

Deng, Weiping; Chen, Jiashu; Kang, Jincan; Zhang, Qinghong; Wang, Ye

2016-05-21

Functionalised carbon nanotube (CNT)-supported Au-Pd alloy nanoparticles were highly efficient catalysts for the aerobic oxidation of amines. We achieved the highest turnover frequencies (>1000 h(-1)) for the oxidative homocoupling of benzylamine and the oxidative dehydrogenation of dibenzylamine. We discovered a cooperative effect between Au-Pd nanoparticles and ketone/quinone groups on CNTs.

Ni Catalysts Supported on Modified Alumina for Diesel Steam Reforming

Directory of Open Access Journals (Sweden)

Antonios Tribalis

2016-01-01

Full Text Available Nickel catalysts are the most popular for steam reforming, however, they have a number of drawbacks, such as high propensity toward coke formation and intolerance to sulfur. In an effort to improve their behavior, a series of Ni-catalysts supported on pure and La-, Ba-, (La+Ba- and Ce-doped γ-alumina has been prepared. The doped supports and the catalysts have been extensively characterized. The catalysts performance was evaluated for steam reforming of n-hexadecane pure or doped with dibenzothiophene as surrogate for sulphur-free or commercial diesel, respectively. The undoped catalyst lost its activity after 1.5 h on stream. Doping of the support with La improved the initial catalyst activity. However, this catalyst was completely deactivated after 2 h on stream. Doping with Ba or La+Ba improved the stability of the catalysts. This improvement is attributed to the increase of the dispersion of the nickel phase, the decrease of the support acidity and the increase of Ni-phase reducibility. The best catalyst of the series doped with La+Ba proved to be sulphur tolerant and stable for more than 160 h on stream. Doping of the support with Ce also improved the catalytic performance of the corresponding catalyst, but more work is needed to explain this behavior.

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.

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.

Multi-wall carbon nanotubes supported molybdenyl acetylacetonate: Efficient and highly reusable catalysts for epoxidation of alkenes with tert-butyl hydroperoxide

Energy Technology Data Exchange (ETDEWEB)

Esnaashari, Fariba [Department of Chemistry, Catalysis Division, University of Isfahan, Isfahan 81746-73441 (Iran, Islamic Republic of); Moghadam, Majid, E-mail: moghadamm@sci.ui.ac.ir [Department of Chemistry, Catalysis Division, University of Isfahan, Isfahan 81746-73441 (Iran, Islamic Republic of); Mirkhani, Valiollah, E-mail: mirkhani@sci.ui.ac.ir [Department of Chemistry, Catalysis Division, University of Isfahan, Isfahan 81746-73441 (Iran, Islamic Republic of); Tangestaninejad, Shahram; Mohammadpoor-Baltork, Iraj; Khosropour, Ahmad Reza; Zakeri, Maryam [Department of Chemistry, Catalysis Division, University of Isfahan, Isfahan 81746-73441 (Iran, Islamic Republic of)

2012-11-15

Efficient epoxidation of olefins catalyzed by MoO{sub 2}(acac){sub 2} supported on amines functionalized MWCNTs is reported. The MWCNTs bearing carboxylic acid groups were modified with 2-aminophenol and 2-aminothiophenol. These amine-MWCNTs act as bidentate ligand for attachment of Mo catalyst. These catalysts were characterized by elemental analysis, scanning electron microscopy, FT-IR and diffuse reflectance UV-Vis spectroscopic methods. The prepared catalysts were used for efficient epoxidation of different alkenes such as cyclic and linear ones with tert-butyl hydroperoxide in refluxing 1,2-dichloroethane. These heterogeneous catalysts can be reused several times without significant loss of their catalytic activity. Highlights: Black-Right-Pointing-Pointer Supporting of molybdenyl acetylacetonate on amine-modified MWCNTs. Black-Right-Pointing-Pointer Heterogeneous catalysts were prepared. Black-Right-Pointing-Pointer These catalysts were highly efficient in the epoxidation of alkenes with TBHP. Black-Right-Pointing-Pointer Makes the catalysts reusable.

Ni-CeO2/C Catalysts with Enhanced OSC for the WGS Reaction

Directory of Open Access Journals (Sweden)

Laura Pastor-Pérez

2015-03-01

Full Text Available In this work, the WGS performance of a conventional Ni/CeO2 bulk catalyst is compared to that of a carbon-supported Ni-CeO2 catalyst. The carbon-supported sample resulted to be much more active than the bulk one. The higher activity of the Ni-CeO2/C catalyst is associated to its oxygen storage capacity, a parameter that strongly influences the WGS behavior. The stability of the carbon-supported catalyst under realistic operation conditions is also a subject of this paper. In summary, our study represents an approach towards a new generation of Ni-ceria based catalyst for the pure hydrogen production via WGS. The dispersion of ceria nanoparticles on an activated carbon support drives to improved catalytic skills with a considerable reduction of the amount of ceria in the catalyst formulation.

The application of inelastic neutron scattering to investigate the steam reforming of methane over an alumina-supported nickel catalyst

International Nuclear Information System (INIS)

McFarlane, Andrew R.; Silverwood, Ian P.; Norris, Elizabeth L.; Ormerod, R. Mark; Frost, Christopher D.; Parker, Stewart F.; Lennon, David

2013-01-01

Highlights: • Inelastic neutron scattering has been used to investigate a Ni/alumina catalyst. • The extent of hydrogen retention by the catalyst has been determined. • Filamentous carbon is identified as a by-product. - Abstract: An alumina-supported nickel catalyst, previously used in methane reforming experiments employing CO 2 as the oxidant, is applied here in the steam reforming variant of the process. Micro-reactor experiments are used to discern an operational window compatible with sample cells designed for inelastic neutron scattering (INS) experiments. INS spectra are recorded after 6 h reaction of a 1:1 mixture of CH 4 and H 2 O at 898 K. Weak INS spectra are observed, indicating minimal hydrogen retention by the catalyst in this operational regime. Post-reaction, the catalyst is further characterised by powder X-ray diffraction, transmission electron microscopy and Raman scattering. In a comparable fashion to that seen for the ‘dry’ reforming experiments, the catalyst retains substantial quantities of carbon in the form of filamentous coke. The role for hydrogen incorporation by the catalyst is briefly considered

The application of inelastic neutron scattering to investigate the steam reforming of methane over an alumina-supported nickel catalyst

Energy Technology Data Exchange (ETDEWEB)

McFarlane, Andrew R.; Silverwood, Ian P. [School of Chemistry, Joseph Black Building, University of Glasgow, Glasgow G12 8QQ (United Kingdom); Norris, Elizabeth L.; Ormerod, R. Mark [Department of Chemistry, School of Physical and Geographical Sciences, Keele University, Staffs ST5 5BG (United Kingdom); Frost, Christopher D.; Parker, Stewart F. [ISIS Facility, STFC Rutherford Appleton Laboratory, Chilton, Didcot, Oxon OX11 0QX (United Kingdom); Lennon, David, E-mail: David.Lennon@glasgow.ac.uk [School of Chemistry, Joseph Black Building, University of Glasgow, Glasgow G12 8QQ (United Kingdom)

2013-12-12

Highlights: • Inelastic neutron scattering has been used to investigate a Ni/alumina catalyst. • The extent of hydrogen retention by the catalyst has been determined. • Filamentous carbon is identified as a by-product. - Abstract: An alumina-supported nickel catalyst, previously used in methane reforming experiments employing CO{sub 2} as the oxidant, is applied here in the steam reforming variant of the process. Micro-reactor experiments are used to discern an operational window compatible with sample cells designed for inelastic neutron scattering (INS) experiments. INS spectra are recorded after 6 h reaction of a 1:1 mixture of CH{sub 4} and H{sub 2}O at 898 K. Weak INS spectra are observed, indicating minimal hydrogen retention by the catalyst in this operational regime. Post-reaction, the catalyst is further characterised by powder X-ray diffraction, transmission electron microscopy and Raman scattering. In a comparable fashion to that seen for the ‘dry’ reforming experiments, the catalyst retains substantial quantities of carbon in the form of filamentous coke. The role for hydrogen incorporation by the catalyst is briefly considered.

CO methanation over supported bimetallic Ni-Fe catalysts: From computational studies towards catalyst optimization

DEFF Research Database (Denmark)

Kustov, Arkadii; Frey, Anne Mette; Larsen, Kasper Emil

2007-01-01

with compositions 25Fe75Ni and 50Fe50Ni showed significantly better activity and in some cases also a higher selectivity to methane compared with the traditional monometallic Ni and Fe catalysts. A catalyst with composition 25Fe75Ni was found to be the most active in CO hydrogenation for the MgAl2O4 support at low...... metal loadings. At high metal concentrations, the maximum for the methanation activity was found for catalysts with composition 50Ni50Fe both on the MgAl2O4 and Al2O3 supports. This difference can be attributed to a higher reducibility of the constituting metals with increasing metal concentration......DFT calculations combined with a computational screening method have previously shown that bimetallic Ni-Fe alloys should be more active than the traditional Ni-based catalyst for CO methanation. That was confirmed experimentally for a number of bimetallic Ni-Fe catalysts supported on MgAl2O4. Here...

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.

CH{sub 4} reforming with CO{sub 2} for syngas production over nickel catalysts supported on mesoporous nanostructured γ-Al{sub 2}O{sub 3}

Energy Technology Data Exchange (ETDEWEB)

Majidian, Nasrollah; Habibi, Narges [Islamic Azad University, Tehran (Iran, Islamic Republic of); Rezaei, Mehran [University of Kashan, Kashan (Iran, Islamic Republic of)

2014-07-15

Nanostructured γ-Al{sub 2}O{sub 3} with high surface area and mesoporous structure was synthesized by sol-gel method and employed as catalyst support for nickel catalysts in methane reforming with carbon dioxide. The prepared samples were characterized by XRD, BET, TPR, TPH, SEM and TPO techniques. The BET analysis showed a high surface area of 204m{sup 2}g{sup -1} and a narrow pore-size distribution centered at a diameter of 5.5 nm for catalyst support. The results revealed that an increase in nickel loading from 5 to 15 wt% decreased the surface area of catalyst from 182 to 160 m{sup 2}g{sup -1}. In addition, the catalytic results showed an increase in methane conversion with increase in nickel content. TPO analysis revealed that the coke deposition increased with increasing in nickel loading, and the catalyst with 15 wt% of nickel showed the highest degree of carbon formation. SEM and TPH analyses confirmed the formation of whisker type carbon over the spent catalysts. Increasing CO{sub 2}/CH{sub 4} ratio increased the methane conversion. The BET analysis of spent catalysts indicated that the mesoporous structure of catalysts still remained after reaction.

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.)

The structure and function of supported molybdenum nitride and molybdenum carbide hydrotreating catalysts

Science.gov (United States)

Dolce, Gregory Martin

1997-11-01

A series of gamma-Alsb2Osb3 supported molybdenum nitrides and carbides were prepared by the temperature programmed reaction of supported molybdates with ammonia and methane/hydrogen mixtures, respectively. In the first part of this research, the effects of synthesis heating rates and molybdenum loading on the catalytic properties of the materials were examined. A significant amount of excess carbon was deposited on the surface of the carbides during synthesis. The materials consisted of small particles which were very highly dispersed. Oxygen chemisorption indicated that the nitride particles may have been two-dimensional. The dispersion of the carbides, however, appeared to decrease as the loading increased. The catalysts were evaluated for hydrodenitrogenation (HDN), hydrodesulfurization (HDS), and hydrodeoxygenation (HDO). The molybdenum loading had the largest effect on the activity of the materials. For the nitrides, the HDN and HDS activities were inverse functions of the loading. This suggested that the most active HDN and HDS sites were located at the perimeter of the two-dimensional particles. The HDN and HDS activities of the carbides followed the same trend as the oxygen uptake. This result suggested that oxygen titrated the active sites on the supported carbides. Selected catalysts were evaluated for methylcarbazole HDN, dibenzothiophene HDS, and dibenzofuran HDO. The activity and selectivity of the nitrides and carbides were competitive with a presulfided commercial catalyst. In the second part of this work, a series of supported nitrides and carbides were prepared using a wider range of loadings (5-30 wt% Mo). Thermogravimetric analysis was used to determine the temperature at which excess carbon was deposited on the carbides. By modifying the synthesis parameters, the deposition of excess carbon was effectively inhibited. The dispersions of the supported nitrides and carbides were constant and suggested that the materials consisted of two

High quality bio-oil from catalytic flash pyrolysis of lignocellulosic biomass over alumina-supported sodium carbonate

KAUST Repository

Imran, Ali; Bramer, Eddy A.; Seshan, Kulathuiyer; Brem, Gerrit

2014-01-01

Performance of a novel alumina-supported sodium carbonate catalyst was studied to produce a valuable bio-oil from catalytic flash pyrolysis of lignocellulosic biomass. Post treatment of biomass pyrolysis vapor was investigated in a catalyst fixed

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

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.

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....

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

Supported chromium-molybdenum and tungsten sulfide catalysts

International Nuclear Information System (INIS)

Chianelli, R.R.; Jacobson, A.J.; Young, A.R.

1988-01-01

This patent describes the process for preparing a supported hydroprocessing catalyst. The process comprising compositing a quantity of a particulate, porous catalyst support material comprising one or more refactory oxides with one or more catalyst precursor salts and heating the composite at elevated temperature of at least about 200/sup 0/C up to about 600/sup 0/, in the presence of a sulfur-bearing compound in an amount whereby sulfur in the form of the sulfur-bearing compound in an amount whereby sulfur in the form of the sulfur bearing compound is present in excess of that contained in the catalyst precursor and under oxygen-free conditions for a time sufficient to form the catalyst. The catalyst precursor salt contains a tetrathiometallate anion of Mo, W or mixture therof and a cation comprising trivalent chromium or a mixture of trivalent chromium with one or more divalent promoter metals selected from the group consisting of Fe, Ni, Co, Mn, Cu and a mixture thereof wherein the trivalent chromium and divalent promoter metals are chelated by at least one neutral, nitrogen-containing polydentate ligand, L

3D Analysis of Fuel Cell Electrocatalyst Degradation on Alternate Carbon Supports.

Science.gov (United States)

Sneed, Brian T; Cullen, David A; Reeves, Kimberly S; Dyck, Ondrej E; Langlois, David A; Mukundan, Rangachary; Borup, Rodney L; More, Karren L

2017-09-06

Understanding the mechanisms associated with Pt/C electrocatalyst degradation in proton exchange membrane fuel cell (PEMFC) cathodes is critical for the future development of higher-performing materials; however, there is a lack of information regarding Pt coarsening under PEMFC operating conditions within the cathode catalyst layer. We report a direct and quantitative 3D study of Pt dispersions on carbon supports (high surface area carbon (HSAC), Vulcan XC-72, and graphitized carbon) with varied surface areas, graphitic character, and Pt loadings ranging from 5 to 40 wt %. This is accomplished both before and after catalyst-cycling accelerated stress tests (ASTs) through observations of the cathode catalyst layer of membrane electrode assemblies. Electron tomography results show Pt nanoparticle agglomeration occurs predominantly at junctions and edges of aggregated graphitized carbon particles, leading to poor Pt dispersion in the as-prepared catalysts and increased coalescence during ASTs. Tomographic reconstructions of Pt/HSAC show much better initial Pt dispersions, less agglomeration, and less coarsening during ASTs in the cathode. However, a large loss of the electrochemically active surface area (ECSA) is still observed and is attributed to accelerated Pt dissolution and nanoparticle coalescence. Furthermore, a strong correlation between Pt particle/agglomerate size and measured ECSA is established and is proposed as a more useful metric than average crystallite size in predicting degradation behavior across different catalyst systems.

Nanostructured carbon-supported Pd electrocatalysts for ethanol oxidation: synthesis and characterization

Science.gov (United States)

Gacutan, E. M.; Climaco, M. I.; Telan, G. J.; Malijan, F.; Hsu, H. Y.; Garcia, J.; Fulo, H.; Tongol, B. J.

2012-12-01

The need to lower the construction cost of fuel cells calls for the development of non-Pt based electrocatalysts. Among others, Pd has emerged as a promising alternative to Pt for fuel cell catalysis. This research aims to investigate the synthesis and characterization of nanostructured Pd-based catalysts dispersed on carbon support as anode materials in direct ethanol fuel cells. For the preparation of the first Pd-based electrocatalyst, palladium nanoparticles (NPs) were synthesized via oleylamine (OAm)-mediated synthesis and precursor method with a mean particle size of 3.63 ± 0.59 nm as revealed by transmission electron microscopy (TEM). Carbon black was used as a supporting matrix for the OAm-capped Pd NPs. Thermal annealing and acetic acid washing were used to remove the OAm capping agent. To evaluate the electrocatalytic activity of the prepared electrocatalyst towards ethanol oxidation, cyclic voltammetry (CV) studies were performed using 1.0 M ethanol in basic medium. The CV data revealed the highest peak current density of 11.05 mA cm-2 for the acetic acid-washed Pd/C electrocatalyst. Meanwhile, the fabrication of the second Pd-based electrocatalyst was done by functionalization of the carbon black support using 3:1 (v/v) H2SO4:HNO3. The metal oxide, NiO, was deposited using precipitation method while polyol method was used for the deposition of Pd NPs. X-ray diffraction (XRD) analysis revealed that the estimated particle size of the synthesized catalysts was at around 9.0-15.0 nm. CV results demonstrated a 36.7% increase in the catalytic activity of Pd-NiO/C (functionalized) catalyst towards ethanol oxidation compared to the non-functionalized catalyst.

Highly Active, Carbon-supported, PdSn Nano-core, Partially ...

African Journals Online (AJOL)

Carbon-supported, Pt partially covered, PdSn alloy nanoparticles (Pt-PdSn/C) were synthesized via a metathetical reaction of PdSn alloy nanoparticles, and a platinum precursor. The electrochemical activity was evaluated by methanol oxidation. The Pt-PdSn/C catalysts were characterized by transmission electron ...

Ruthenium-platinum bimetallic catalysts supported on silica: characterization and study of benzene hydrogenation and CO methanation

Energy Technology Data Exchange (ETDEWEB)

Chakrabarty, D.K.; Rao, K.M.; Sundararaman, N.; Chandavar, K.

1986-12-15

Ru-Pt/SiO/sub 2/ bimetallic catalysts with varying Ru:Pt ratio have been prepared and studied with the aim to establish if they contain coclusters or isolated ruthenium and platinum particles. X-ray diffraction studies show that individual crystallites of ruthenium and platinum are present and no coclusters are formed. Metal dispersion has been determined by hydrogen chemisorption and surface composition of the catalysts has been obtained from XPS. It was found that preoxidation of the catalysts prior to reduction is essential for good platinum dispersion. The experimental turnover number (TN) for benzene hydrogenation on the bimetallic catalysts agrees very well with that of the weighted average on the individual metal catalysts and this may be taken as a kinetic evidence for the absence of coclusters. Carbon monoxide methanation activity of the bimetallic catalysts is quite similar to that of the supported platinum catalyst. 6 refs., 6 figs., 2 tabs.

Carbon-Supported Fe Catalysts for CO2 Electroreduction to High-Added Value Products: A DEMS Study: Effect of the Functionalization of the Support

OpenAIRE

Pérez-Rodríguez, S.; García, G.; Calvillo, L.; Celorrio, V.; Pastor, E.; Lázaro, M. J.

2011-01-01

Vulcan XC-72R-supported Fe catalysts have been synthesised for the electroreduction of CO2 to high-added value products. Catalysts were obtained by the polyol method, using ethylene glycol as solvent and reducing agent. Prior to the metal deposition, Vulcan was subjected to different oxidation treatments in order to modify its surface chemistry and study its influence on the physicochemical and electrochemical properties of the catalysts, as well as on the product distribution. The oxidation ...

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.

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)

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.

Polymer-Supported Raney Nickel Catalysts for Sustainable Reduction Reactions

Directory of Open Access Journals (Sweden)

Haibin Jiang

2016-06-01

Full Text Available Green is the future of chemistry. Catalysts with high selectivity are the key to green chemistry. Polymer-supported Raney catalysts have been found to have outstanding performance in the clean preparation of some chemicals. For example, a polyamide 6-supported Raney nickel catalyst provided a 100.0% conversion of n-butyraldehyde without producing any detectable n-butyl ether, the main byproduct in industry, and eliminated the two main byproducts (isopropyl ether and methyl-iso-butylcarbinol in the hydrogenation of acetone to isopropanol. Meanwhile, a model for how the polymer support brought about the elimination of byproducts is proposed and confirmed. In this account the preparation and applications of polymer-supported Raney catalysts along with the corresponding models will be reviewed.

High Performance Nanocatalysts Supported on Micro/Nano Carbon Structures Using Ethanol Immersion Pretreatment for Micro DMFCs

International Nuclear Information System (INIS)

Lin, Liang-You; Wu, Yi-Shiuan; Chang, Chaun; Tseng, Fan-Gang

2013-01-01

In this paper, highly dense platinum (Pt) nanocatalysts were successfully deposited on the hydrophilically-treated nano/micro carbon supports with an ethanol (EtOH) immersion pretreatment and an acidic treatment for the performance improvement of methanol oxidation reaction (MOR). In order to thoroughly immerse the three-dimensional, interwoven structures of the carbon cloth fibers with a 6 M sulfuric acid surface modification, which increasing more oxygen-containing functional groups on the surfaces of the carbon supports, the EtOH immersion pretreatment of the carbon supports was utilized prior to the sulfuric acid treatment. Subsequently, Pt catalysts were reduced on the modified carbon supports by a homemade open-loop reduction system (OLRS) [1] For comparisons, carbon cloth (CC) and carbon nanotube on CC (CNT/CC) supports were employed with and without EtOH immersion pretreatments before Pt catalyst reduction. In the cyclic voltammetry (CV) curves, the electrosorption charges of hydrogen ion (Q H ) and the peak current density (I P ) of the fabricated Pt/CC and Pt/CNT/CC electrodes with the EtOH immersion pretreatments can efficiently be enhanced due to more active Pt sites for electrocatalytic reactions

Heterogenization of Homogeneous Catalysts: the Effect of the Support

Energy Technology Data Exchange (ETDEWEB)

Earl, W.L.; Ott, K.C.; Hall, K.A.; de Rege, F.M.; Morita, D.K.; Tumas, W.; Brown, G.H.; Broene, R.D.

1999-06-29

We have studied the influence of placing a soluble, homogeneous catalyst onto a solid support. We determined that such a 'heterogenized' homogeneous catalyst can have improved activity and selectivity for the asymmetric hydrogenation of enamides to amino acid derivatives. The route of heterogenization of RhDuPhos(COD){sup +} cations occurs via electrostatic interactions with anions that are capable of strong hydrogen bonding to silica surfaces. This is a novel approach to supported catalysis. Supported RhDuPhos(COD){sup +} is a recyclable, non-leaching catalyst in non-polar media. This is one of the few heterogenized catalysts that exhibits improved catalytic performance as compared to its homogeneous analog.

57Fe Moessbauer Studies in Mo-Fe Supported Catalysts

International Nuclear Information System (INIS)

Castelao-Dias, M.; Costa, B. F. O.; Quinta-Ferreira, R. M.

2001-01-01

Industrially, the Mo-Fe catalysts used in the selective oxidation of methanol to formaldehyde can rapidly deactivate. The use of support materials may reduce the high temperatures in the catalytic bed and/or increase thermal and mechanical resistance. However, during the preparation of these catalysts, or even during reaction conditions, the active species may react with the support material losing their catalytic activity. In this work silica, silicium carbide and titania were studied as supported catalysts by Moessbauer spectroscopy which proved to be a useful technique in the choice of supported materials

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.

Nanostructured Carbon Materials as Supports in the Preparation of Direct Methanol Fuel Cell Electrocatalysts

Directory of Open Access Journals (Sweden)

María Jesús Lázaro

2013-08-01

Full Text Available Different advanced nanostructured carbon materials, such as carbon nanocoils, carbon nanofibers, graphitized ordered mesoporous carbons and carbon xerogels, presenting interesting features such as high electrical conductivity and extensively developed porous structure were synthesized and used as supports in the preparation of electrocatalysts for direct methanol fuel cells (DMFCs. The main advantage of these supports is that their physical properties and surface chemistry can be tailored to adapt the carbonaceous material to the catalytic requirements. Moreover, all of them present a highly mesoporous structure, diminishing diffusion problems, and both graphitic character and surface area can be conveniently modified. In the present work, the influence of the particular features of each material on the catalytic activity and stability was analyzed. Results have been compared with those obtained for commercial catalysts supported on Vulcan XC-72R, Pt/C and PtRu/C (ETEK. Both a highly ordered graphitic and mesopore-enriched structure of these advanced nanostructured materials resulted in an improved electrochemical performance in comparison to the commercial catalysts assayed, both towards CO and alcohol oxidation.

Influence of pore structure and chemical properties of supported Mo catalysts on their performance in upgrading heavy coal liquids

Energy Technology Data Exchange (ETDEWEB)

Song, C.; Hanaoka, K.; Nomura, M. (Pennsylvania State University, University Park, PA (USA). Dept. of Materials Science and Engineering)

In the hydroprocessing of solvent-refined coals, both the pore structure and the chemical properties of the catalysts affect the conversion of the heavy materials. Increasing median pore diameter (MPD) of unimodal Ni-Mo/Al[sub 2]O[sub 3] catalysts in the relatively small pore region (up to 150 [angstrom]) enhanced the conversion of both asphaltene and preasphaltene, but further increasing the MPD up to 730 [angstrom] mainly promoted preasphaltene conversion. In the runs of the isolated fractions, however, conversions increased with MPD up to 290 [angstrom] for asphaltene and up to 730 [angstrom] for preasphaltene. The degree of heteroatom removal is also influenced by MPD. There exist preferable pore size ranges for hydrodeoxygenation. Two Mo/SiO[sub 2] and several carbon-coated Ni-Mo/Al[sub 2]O[sub 3] catalysts with different MPD and a commercial Ni-Mo supported on silicated Al[sub 2]O[sub 3] were also compared. The increasing MPD of SiO[sub 2]-supported Mo catalysts increased the conversion of preasphaltene materials. Mo/SiO[sub 2] catalysts are more effective than Ni-Mo supported on Al[sub 2]O[sub 3] and silicated Al[sub 2]O[sub 3] for converting preasphaltene materials, while the latter two are more active for conversion of asphaltene into oil. Another interesting observation is that, for a given MPD range, the carbon-coated Ni-Mo/Al[sub 2]O[sub 3] catalysts gave higher preasphaltene conversions than fresh ones. These results point to the conclusion that larger pore and less acidic hydrogenation catalysts are more effective for preasphaltene conversion, but efficient conversion of asphaltene into oil is facilitated by mild hydrocracking catalysts having appropriate pore size ranges. 43 refs., 8 figs., 9 tabs.

One-step liquid phase chemical method to prepare carbon-based amorphous molybdenum sulfides: As the effective hydrogen evolution reaction catalysts

International Nuclear Information System (INIS)

Guo, Mengmeng; Wu, Qikang; Yu, Miaomiao; Wang, Yinling; Li, Maoguo

2017-01-01

Two different kinds of carbon-based amorphous molybdenum sulfide composite catalysts (activated carbon supported amorphous molybdenum sulfide and acetylene black supported amorphous molybdenum sulfide) had been prepared in a facile and scalable one-step liquid phase chemical method. The morphological and structural information of catalysts was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-Ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and it’s electro-catalytic HER activity were evaluated by linear sweep voltammetry(LSV), amperometric i-t technology and AC impedance technology. The as-prepared carbon-based amorphous molybdenum sulfides showed greatly enhanced electro-catalytic activity for HER compared with pure amorphous molybdenum sulfides. Especially, the nano-sized acetylene black supported molybdenum sulfide exhibited excellent electro-catalytic HER performances with a low onset potential of −116 mV versus reverse hydrogen electrode (RHE) and a small Tafel slope of 51 mV per decade.

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.

Polypropylene obtained through zeolite supported catalysts

Directory of Open Access Journals (Sweden)

Queli C. Bastos

2004-01-01

Full Text Available Propylene polymerizations were carried out with f2C(Flu(CpZrCl2 and SiMe2(Ind2ZrCl2 catalysts supported on silica, zeolite sodic mordenite (NaM and acid mordenite (HM. The polymerizations were performed at different temperatures and varying aluminium/zirconium molar ratios ([Al]/[Zr]. The effect of these reaction parameters on the catalyst activity was investigated using a proposed statistical experimental planning. In the case of f2C(Flu(CpZrCl2, SiO2 and NaM were used as support and the catalyst performance evaluated using toluene and pentane as polymerization solvent. The molecular weight, molecular weight distribution, melting point and crystallinity of the polymers were examined. The results indicate very high activities for the syndiospecific heterogeneous system. Also, the polymers obtained had superior Mw and stereoregularity.

Polypropylene obtained through zeolite supported catalysts

International Nuclear Information System (INIS)

Bastos, Queli C.; Marques, Maria de Fatima V.

2004-01-01

Propylene polymerizations were carried out with φ 2 C(Flu)(Cp)ZrCl 2 and SiMe 2 (Ind)2ZrCl 2 catalysts supported on silica, zeolite sodic mordenite (NaM) and acid mordenite (HM). The polymerizations were performed at different temperatures and varying aluminium/zirconium molar ratios ([Al]/[Zr]). The effect of these reaction parameters on the catalyst activity was investigated using a proposed statistical experimental planning. In the case of f 2 C(Flu)(Cp)ZrCl 2 , SiO 2 and NaM were used as support and the catalyst performance evaluated using toluene and pentane as polymerization solvent. The molecular weight, molecular weight distribution, melting point and crystallinity of the polymers were examined. The results indicate very high activities for the syndiospecific heterogeneous system. Also, the polymers obtained had superior Mw and stereo regularity. (author)

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.

Propene Hydroformylation by Supported Aqueous-phase Rh-NORBOS Catalysts

DEFF Research Database (Denmark)

Riisager, Anders; Eriksen, Kim Michael; Hjortkjær, Jes

2003-01-01

The gas-phase hydroformylation reaction of propene using supported aqueous-phase (SAP) Rh-NORBOS modified catalysts in a continuous flow reactor has been examined. SAP catalysts supported on six different support materials were made by wet impregnation using solutions of the precursor complex Rh(...

Catalyst support effects on hydrogen spillover

Science.gov (United States)

Karim, Waiz; Spreafico, Clelia; Kleibert, Armin; Gobrecht, Jens; Vandevondele, Joost; Ekinci, Yasin; van Bokhoven, Jeroen A.

2017-01-01

Hydrogen spillover is the surface migration of activated hydrogen atoms from a metal catalyst particle, on which they are generated, onto the catalyst support. The phenomenon has been much studied and its occurrence on reducible supports such as titanium oxide is established, yet questions remain about whether hydrogen spillover can take place on nonreducible supports such as aluminium oxide. Here we use the enhanced precision of top-down nanofabrication to prepare controlled and precisely tunable model systems that allow us to quantify the efficiency and spatial extent of hydrogen spillover on both reducible and nonreducible supports. We place multiple pairs of iron oxide and platinum nanoparticles on titanium oxide and aluminium oxide supports, varying the distance between the pairs from zero to 45 nanometres with a precision of one nanometre. We then observe the extent of the reduction of the iron oxide particles by hydrogen atoms generated on the platinum using single-particle in situ X-ray absorption spectromicroscopy applied simultaneously to all particle pairs. The data, in conjunction with density functional theory calculations, reveal fast hydrogen spillover on titanium oxide that reduces remote iron oxide nanoparticles via coupled proton-electron transfer. In contrast, spillover on aluminium oxide is mediated by three-coordinated aluminium centres that also interact with water and that give rise to hydrogen mobility competing with hydrogen desorption; this results in hydrogen spillover about ten orders of magnitude slower than on titanium oxide and restricted to very short distances from the platinum particle. We anticipate that these observations will improve our understanding of hydrogen storage and catalytic reactions involving hydrogen, and that our approach to creating and probing model catalyst systems will provide opportunities for studying the origin of synergistic effects in supported catalysts that combine multiple functionalities.

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

DEFF Research Database (Denmark)

Andersen, Shuang Ma; Skou, Eivind Morten

2014-01-01

Significant differences in catalyst performance and durability are often observed between the use of a liquid electrolyte (e.g. sulfuric acid), and a solid polymer electrolyte (e.g. Nafion®). To understand this phenomenon, we studied the electrochemical behavior of a commercially available carbon...

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)

An oxidation-resistant indium tin oxide catalyst support for proton exchange membrane fuel cells

Energy Technology Data Exchange (ETDEWEB)

Chhina, H.; Campbell, S. [Ballard Power Systems Inc., 9000 Glenlyon Parkway, Burnaby, BC V5J 5J8 (Canada); Kesler, O. [Department of Mechanical Engineering, University of British Columbia, Vancouver, BC, V6T 1Z4 (Canada)

2006-10-27

The oxidation of carbon catalyst supports causes degradation in catalyst performance in proton exchange membrane fuel cells (PEMFCs). Indium tin oxide (ITO) is considered as a candidate for an alternative catalyst support. The electrochemical stability of ITO was studied by use of a rotating disk electrode (RDE). Oxidation cycles between +0.6 and +1.8V were applied to ITO supporting a Pt catalyst. Cyclic voltammograms (CVs) both before and after the oxidation cycles were obtained for Pt on ITO, Hispec 4000 (a commercially available catalyst), and 40wt.% Pt dispersed in-house on Vulcan XC-72R. Pt on ITO showed significantly better electrochemical stability, as determined by the relative change in electrochemically active surface area after cycling. Hydrogen desorption peaks in the CVs existed even after 100 cycles from 0.6 to 1.8V for Pt on ITO. On the other hand, most of the active surface area was lost after 100 cycles of the Hispec 4000 catalyst. The 40wt.% Pt on Vulcan made in-house also lost most of its active area after only 50 cycles. Pt on ITO was significantly more electrochemically stable than both Hispec 4000 and Pt on Vulcan XC-72R. In this study, it was found that the Pt on ITO had average crystallite sizes of 13nm for Pt and 38nm for ITO. Pt on ITO showed extremely high thermal stability, with only {approx}1wt.% loss of material for ITO versus {approx}57wt.% for Hispec 4000 on heating to 1000{sup o}C. The TEM data show Pt clusters dispersed on small crystalline ITO particles. The SEM data show octahedral shaped ITO particles supporting Pt. (author)

SiC nanocrystals as Pt catalyst supports for fuel cell applications

DEFF Research Database (Denmark)

Dhiman, Rajnish; Morgen, Per; Skou, E.M.

2013-01-01

A robust catalyst support is pivotal to Proton Exchange Membrane Fuel Cells (PEMFCs) to overcome challenges such as catalyst support corrosion, low catalyst utilization and overall capital cost. SiC is a promising candidate material which could be applied as a catalyst support in PEMFCs. Si...... on the nanocrystals of SiC-SPR and SiC-NS by the polyol method. The SiC substrates are subjected to an acid treatment to introduce the surface groups, which help to anchor the Pt nano-catalysts. These SiC based catalysts have been found to have a higher electrochemical activity than commercially available Vulcan...... based catalysts (BASF & HISPEC). These promising results signal a new era of SiC based catalysts for fuel cell applications....

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...

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...

Attrition Resistant Fischer-Tropsch Catalysts Based on FCC Supports

Energy Technology Data Exchange (ETDEWEB)

Adeyiga, Adeyinka

2010-02-05

Commercial spent fluid catalytic cracking (FCC) catalysts provided by Engelhard and Albemarle were used as supports for Fe-based catalysts with the goal of improving the attrition resistance of typical F-T catalysts. Catalysts with the Ruhrchemie composition (100 Fe/5 Cu/4.2 K/25 spent FCC on mass basis) were prepared by wet impregnation. XRD and XANES analysis showed the presence of Fe{sub 2}O{sub 3} in calcined catalysts. FeC{sub x} and Fe{sub 3}O{sub 4} were present in the activated catalysts. The metal composition of the catalysts was analyzed by ICP-MS. F-T activity of the catalysts activated in situ in CO at the same conditions as used prior to the attrition tests was measured using a fixed bed reactor at T = 573 K, P = 1.38 MPa and H{sub 2}:CO ratio of 0.67. Cu and K promoted Fe supported over Engelhard provided spent FCC catalyst shows relatively good attrition resistance (8.2 wt% fines lost), high CO conversion (81%) and C{sub 5}+ hydrocarbons selectivity (18.3%).

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.

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.

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

Science.gov (United States)

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

2016-02-01

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

Zircon Supported Copper Catalysts for the Steam Reforming of Methanol

Science.gov (United States)

Widiastri, M.; Fendy, Marsih, I. N.

2008-03-01

Steam reforming of methanol (SRM) is known as one of the most favorable catalytic processes for producing hydrogen. Current research on zirconia, ZrO2 supported copper catalyst revealed that CuO/ZrO2 as an active catalyst for the SRM. Zircon, ZrSiO4 is available from the by-product of tin mining. In the work presented here, the catalytic properties of CuO/ZrSiO4 with various copper oxide compositions ranging from 2.70% (catalyst I), 4.12% (catalyst II), and 7.12%-mass (catalyst III), synthesized by an incipient wetness impregnation technique, were investigated to methanol conversion, selectivity towards CO formation, and effect of ZnO addition (7.83%CuO/8.01%ZnO/ZrSiO4 = catalyst V). The catalytic activity was obtained using a fixed bed reactor and the zircon supported catalyst activity was compared to those of CuO/ZnO/Al2O3 catalyst (catalyst IV) and commercial Kujang LTSC catalyst. An X-ray powder diffraction (XRD) analysis was done to identify the abundant phases of the catalysts. The catalysts topography and particle diameter were measured with scanning electron microscopy (SEM) and composition of the catalysts was measured by SEM-EDX, scanning electron microscope-energy dispersive using X-ray analysis. The results of this research provide information on the possibility of using zircon (ZrSiO4) as solid support for SRM catalysts.

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.

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.

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.

Support Functionalization To Retard Ostwald Ripening in Copper Methanol Synthesis Catalysts

NARCIS (Netherlands)

van den Berg, Roy; Parmentier, Tanja E.; Elkjaer, Christian F.; Gommes, Cedric J.; Sehested, Jens; Helveg, Stig; de Jongh, Petra E.; de Jong, Krijn P.

A main reason for catalyst deactivation in supported catalysts for methanol synthesis is copper particle growth. We have functionalized the support surface in order to suppress the formation and/or transport of mobile copper species and thereby catalyst deactivation. A Stober silica support was

Hydrogenation of Levulinic Acid to gamma-Valerolactone in Water Using Millimeter Sized Supported Ru Catalysts in a Packed Bed Reactor

NARCIS (Netherlands)

Piskun, A. S.; de Haan, J. E.; Wilbers, E.; de Bovenkamp, H. H. van; Tang, Z.; Heeres, Hero

gamma-Valerolactone (GVL) has been identified as a sustainable platform chemical for the production of carbon-based chemicals. We here report an experimental study on the catalytic hydrogenation of levulinic acid (LA) in water to GVL in a packed bed reactor using supported Ru catalysts (carbon,

A Study of CO2 Methanation over Ni-Based Catalysts Supported by CNTs with Various Textural Characteristics

OpenAIRE

Yanyan Feng; Wen Yang; Wei Chu

2015-01-01

This work studied the influence of textural characteristics of CNTs on catalytic performance of Ni/CNTs for CO2 methanation. The CNTs supports were prepared by chemical vapor deposition method using Ni/MgO catalysts, and acetonitrile and ethanol were used as carbon sources, respectively. The Ni/CNTs catalysts were prepared via impregnation method and characterized by X-ray diffraction (XRD), N2 adsorption/desorption, and temperature-programmed reduction (H2-TPR) techniques. The results indica...

Stability, carbon resistance, and reactivity toward autothermal reforming of nickel on ceria-based supports

International Nuclear Information System (INIS)

Sutthisripok, W.; Laosiripojana, N.

2004-01-01

'Full text:' Solid Oxide Fuel Cell (SOFC) normally requires a reformer unit, where the fuel such as natural gas, methane, methanol, or ethanol can be reformed to hydrogen before introducing to the main part of fuel cell. Nickel on commercial supports such as Al2O3, MgO, ZrO2 has been widely reported to be used as the reforming catalyst commercially. Carbon formation and catalyst deactivation are always the main problems of using this type of catalyst. It is well established that CeO2 and CeO2-ZrO2 have been applied as the catalysts in a wide variety of reactions involving oxidation or partial oxidation of hydrocarbons (e.g. automotive catalysis). In order to quantify the performance of nickel on CeO2 and CeO2-ZrO2 supports for reformer application, the stabilities toward methane steam reforming and the carbon formation resistance were studied. After 18 hours, nickel on CeO2-ZrO2 with the Ce/Zr ratio of 3/1 presented the best performance in term of stability and activity. It also provided excellent resistance toward carbon formation compared to commercial Ni/Al2O3. The autothermal reforming of methane over Ni catalyst on CeO2 and CeO2-ZrO2 supports were also investigated. Ni/Ce-ZrO2 with the Ce/ Zr ratio of 3/1 also showed the best performance. The kinetics of this reaction was also studied. In the temperature range of 750-900C, the reaction order in methane was always closed to 1. The catalyst showed a slight positive effect of hydrogen and a negative effect of steam on the steam reforming rate. The addition of oxygen increased the steam reforming rate. However, the productions of CO and H2 decreased with increasing oxygen partial pressure. (author)

Nanostructured carbon-supported Pd electrocatalysts for ethanol oxidation: synthesis and characterization

International Nuclear Information System (INIS)

Gacutan, E M; Tongol, B J; Climaco, M I; Telan, G J; Malijan, F; Hsu, H Y; Garcia, J; Fulo, H

2012-01-01

The need to lower the construction cost of fuel cells calls for the development of non-Pt based electrocatalysts. Among others, Pd has emerged as a promising alternative to Pt for fuel cell catalysis. This research aims to investigate the synthesis and characterization of nanostructured Pd-based catalysts dispersed on carbon support as anode materials in direct ethanol fuel cells. For the preparation of the first Pd-based electrocatalyst, palladium nanoparticles (NPs) were synthesized via oleylamine (OAm)-mediated synthesis and precursor method with a mean particle size of 3.63 ± 0.59 nm as revealed by transmission electron microscopy (TEM). Carbon black was used as a supporting matrix for the OAm-capped Pd NPs. Thermal annealing and acetic acid washing were used to remove the OAm capping agent. To evaluate the electrocatalytic activity of the prepared electrocatalyst towards ethanol oxidation, cyclic voltammetry (CV) studies were performed using 1.0 M ethanol in basic medium. The CV data revealed the highest peak current density of 11.05 mA cm −2 for the acetic acid-washed Pd/C electrocatalyst. Meanwhile, the fabrication of the second Pd-based electrocatalyst was done by functionalization of the carbon black support using 3:1 (v/v) H 2 SO 4 :HNO 3 . The metal oxide, NiO, was deposited using precipitation method while polyol method was used for the deposition of Pd NPs. X-ray diffraction (XRD) analysis revealed that the estimated particle size of the synthesized catalysts was at around 9.0–15.0 nm. CV results demonstrated a 36.7% increase in the catalytic activity of Pd–NiO/C (functionalized) catalyst towards ethanol oxidation compared to the non-functionalized catalyst. (paper)

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.

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.

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