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.

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

Energy Technology Data Exchange (ETDEWEB)

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

2016-12-01

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

Electrochemical characterization of nano-sized Pd-based catalysts as cathode materials in direct methanol fuel cells.

Science.gov (United States)

Choi, M; Han, C; Kim, I T; An, J C; Lee, J J; Lee, H K; Shim, J

2011-01-01

To improve the catalytic activity of palladium (Pd) as a cathode catalyst in direct methanol fuel cells (DMFCs), we prepared palladium-titanium oxide (Pd-TiO2) catalysts which the Pd and TiO2 nanoparticles were simultaneously impregnated on carbon. We selected Pd and TiO2 as catalytic materials because of their electrochemical stability in acid solution. The crystal structure and the loading amount of Pd and TiO2 on carbon were characterized by X-ray diffraction (XRD) and energy dispersive X-ray microanalysis (EDX). The electrochemical characterization of Pd-TiO2/C catalysts for the oxygen reduction reaction was carried out in half and single cell systems. The catalytic activities of the Pd-TiO2 catalysts were strongly influenced by the TiO2 content. In the single cell test, the Pd-TiO2 catalysts showed very comparable performance to the Pt catalyst.

Direct methanol feed fuel cell with reduced catalyst loading

Science.gov (United States)

Kindler, Andrew (Inventor)

1999-01-01

Improvements to direct feed methanol fuel cells include new protocols for component formation. Catalyst-water repellent material is applied in formation of electrodes and sintered before application of ionomer. A membrane used in formation of an electrode assembly is specially pre-treated to improve bonding between catalyst and membrane. The improved electrode and the pre-treated membrane are assembled into a membrane electrode assembly.

Anode catalysts for direct ethanol fuel cells utilizing directly solar light illumination.

Science.gov (United States)

Chu, Daobao; Wang, Shuxi; Zheng, Peng; Wang, Jian; Zha, Longwu; Hou, Yuanyuan; He, Jianguo; Xiao, Ying; Lin, Huashui; Tian, Zhaowu

2009-01-01

Shine a light: A PtNiRu/TiO(2) anode catalyst for direct ethanol fuel cells shows photocatalytic activity. The peak current density for ethanol oxidation under solar light illumination is 2-3 times greater than that in the absence of solar light. Ethanol is oxidized by light-generated holes, and the electrons are collected by the TiO(2) support to generate the oxidation current.Novel PtNiRu/TiO(2) anode catalysts for direct ethanol fuel cells (DEFCs) were prepared from PtNiRu nanoparticles (1:1:1 atomic ratios) and a nanoporous TiO(2) film by a sol-gel and electrodeposition method. The performances of the catalysts for ethanol oxidation were investigated by cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy. The results indicate a remarkable enhancement of activity for ethanol oxidation under solar light illumination. Under solar light illumination, the generated oxidation peak current density is 24.6 mA cm(-2), which is about 2.5 times higher than that observed without solar light (9.9 mA cm(-2)). The high catalytic activity of the PtNiRu/TiO(2) complex catalyst for the electrooxidation of ethanol may be attributed to the modified metal/nanoporous TiO(2) film, and the enhanced electrooxidation of ethanol under solar light may be due to the photogeneration of holes in the modified nanoporous TiO(2) film.

Study of PtNi/C catalyst for direct ethanol fuel cell

International Nuclear Information System (INIS)

Moraes, L.P.R. de; Silva, E.L. da; Amico, S.C.; Malfatti, C.F.

2014-01-01

In this work, PtNi binary catalyst and pure platin catalyst were synthesized by the impregnation-reduction method, using Vulcan XC72R as support, for direct ethanol fuel cells. The composition and structure of the catalysts were analyzed by X-ray diffraction, the electrochemical behavior was evaluated by cyclic voltammetry and morphology of the catalysts was studied by high-resolution transmission electron microscopy. The results showed that the addition of Ni to Pt led to the contraction of the crystal lattice, increased the catalytic activity compared to pure Pt and initiated the electrooxidation of ethanol at lower potential. (author)

Full Scale Alternative Catalyst Testing for Bosch Reactor Optimization

Science.gov (United States)

Barton, Katherine; Abney, Morgan B.

2011-01-01

Current air revitalization technology onboard the International Space Station (ISS) cannot provide complete closure of the oxygen and hydrogen loops. This makes re-supply necessary, which is possible for missions in low Earth orbit (LEO) like the ISS, but unviable for long term space missions outside LEO. In comparison, Bosch technology reduces carbon dioxide with hydrogen, traditionally over a steel wool catalyst, to create water and solid carbon. The Bosch product water can then be fed to the oxygen generation assembly to produce oxygen for crew members and hydrogen necessary to reduce more carbon dioxide. Bosch technology can achieve complete oxygen loop closure, but has many undesirable factors that result in a high energy, mass, and volume system. Finding a different catalyst with an equal reaction rate at lower temperatures with less catalyst mass and longer lifespan would make a Bosch flight system more feasible. Developmental testing of alternative catalysts for the Bosch has been performed using the Horizontal Bosch Test Stand. Nickel foam, nickel shavings, and cobalt shavings were tested at 500 C and compared to the original catalyst, steel wool. This paper presents data and analysis on the performance of each catalyst tested at comparable temperatures and recycle flow rates.

Nano-Engineered Catalysts for Direct Methanol Fuel Cells

Science.gov (United States)

Myung, Nosang; Narayanan, Sekharipuram; Wiberg, Dean

2008-01-01

Nano-engineered catalysts, and a method of fabricating them, have been developed in a continuing effort to improve the performances of direct methanol fuel cells as candidate power sources to supplant primary and secondary batteries in a variety of portable electronic products. In order to realize the potential for high energy densities (as much as 1.5 W h/g) of direct methanol fuel cells, it will be necessary to optimize the chemical compositions and geometric configurations of catalyst layers and electrode structures. High performance can be achieved when catalyst particles and electrode structures have the necessary small feature sizes (typically of the order of nanometers), large surface areas, optimal metal compositions, high porosity, and hydrophobicity. The present method involves electrodeposition of one or more catalytic metal(s) or a catalytic-metal/polytetrafluoroethylene nanocomposite on an alumina nanotemplate. The alumina nanotemplate is then dissolved, leaving the desired metal or metal/polytetrafluoroethylene-composite catalyst layer. Unlike some prior methods of making fine metal catalysts, this method does not involve processing at elevated temperature; all processing can be done at room temperature. In addition, this method involves fewer steps and is more amenable to scaling up for mass production. Alumina nanotemplates are porous alumina membranes that have been fabricated, variously, by anodizing either pure aluminum or aluminum that has been deposited on silicon by electronbeam evaporation. The diameters of the pores (7 to 300 nm), areal densities of pores (as much as 7 x 10(exp 10)sq cm), and lengths of pores (up to about 100 nm) can be tailored by selection of fabrication conditions. In a given case, the catalytic metal, catalytic metal alloy, or catalytic metal/ polytetrafluoroethylene composite is electrodeposited in the pores of the alumina nanotemplate. The dimensions of the pores, together with the electrodeposition conditions

Methanol-Tolerant Cathode Catalyst Composite For Direct Methanol Fuel Cells

Science.gov (United States)

Zhu, Yimin; Zelenay, Piotr

2006-03-21

A direct methanol fuel cell (DMFC) having a methanol fuel supply, oxidant supply, and its membrane electrode assembly (MEA) formed of an anode electrode and a cathode electrode with a membrane therebetween, a methanol oxidation catalyst adjacent the anode electrode and the membrane, an oxidant reduction catalyst adjacent the cathode electrode and the membrane, comprises an oxidant reduction catalyst layer of a platinum-chromium alloy so that oxidation at the cathode of methanol that crosses from the anode through the membrane to the cathode is reduced with a concomitant increase of net electrical potential at the cathode electrode.

Catalyst inks and method of application for direct methanol fuel cells

Science.gov (United States)

Zelenay, Piotr; Davey, John; Ren, Xiaoming; Gottesfeld, Shimshon; Thomas, Sharon C.

2004-02-24

Inks are formulated for forming anode and cathode catalyst layers and applied to anode and cathode sides of a membrane for a direct methanol fuel cell. The inks comprise a Pt catalyst for the cathode and a Pt--Ru catalyst for the anode, purified water in an amount 4 to 20 times that of the catalyst by weight, and a perfluorosulfonic acid ionomer in an amount effective to provide an ionomer content in the anode and cathode surfaces of 20% to 80% by volume. The inks are prepared in a two-step process while cooling and agitating the solutions. The final solution is placed in a cooler and continuously agitated while spraying the solution over the anode or cathode surface of the membrane as determined by the catalyst content.

Low-Pt-Content Anode Catalyst for Direct Methanol Fuel Cells

Science.gov (United States)

Narayanan, Sekharipuram; Whitacre, Jay

2008-01-01

Combinatorial experiments have led to the discovery that a nanophase alloy of Pt, Ru, Ni, and Zr is effective as an anode catalyst material for direct methanol fuel cells. This discovery has practical significance in that the electronic current densities achievable by use of this alloy are comparable or larger than those obtained by use of prior Pt/Ru catalyst alloys containing greater amounts of Pt. Heretofore, the high cost of Pt has impeded the commercialization of direct methanol fuel cells. By making it possible to obtain a given level of performance at reduced Pt content (and, hence, lower cost), the discovery may lead to reduction of the economic impediment to commercialization.

STUDY OF SOLVENT AND CATALYST INTERACTIONS IN DIRECT COAL LIQUEFACTION; SEMIANNUAL

International Nuclear Information System (INIS)

Michael T. Klein

2000-01-01

There are several aspects of the Direct Coal Liquefaction process which are not fully understood and which if better understood might lead to improved yields and conversions. Among these questions are the roles of the catalyst and the solvent. While the solvent is known to act by transfer of hydrogen atoms to the free radicals formed by thermal breakdown of the coal in an uncatalyzed system, in the presence of a solid catalyst as is now currently practiced, the yields and conversions are higher than in an uncatalyzed system. The role of the catalyst in this case is not completely understood. DOE has funded many projects to produce ultrafine and more active catalysts in the expectation that better contact between catalyst and coal might result. This approach has met with limited success probably because mass transfer between two solids in a fluid medium i.e. the catalyst and the coal, is very poor. It is to develop an understanding of the role of the catalyst and solvent in Direct Liquefaction that this project was initiated. Specifically it was of interest to know whether direct contact between the coal and the catalyst was important. By separating the solid catalyst in a stainless steel basket permeable to the solvent but not the coal in the liquefaction reactor, it was shown that the catalyst still maintains a catalytic effect on the liquefaction process. There is apparently transfer of hydrogen atoms from the catalyst through the basket wall to the coal via the solvent. Strong hydrogen donor solvents appear to be more effective in this respect than weak hydrogen donors. It therefore appears that intimate contact between catalyst and coal is not a requirement, and that the role of the catalyst may be to restore the hydrogen donor strength to the solvent as the reaction proceeds. A range of solvents of varying hydrogen donor strength was investigated. Because of the extensive use of thermogravimetric analysis in this laboratory in was noted that the peak

Mixed phase Pt-Ru catalyst for direct methanol fuel cell anode by flame aerosol synthesis

DEFF Research Database (Denmark)

Chakraborty, Debasish; Bischoff, H.; Chorkendorff, Ib

2005-01-01

A spray-flame aerosol catalyzation technique was studied for producing Pt-Ru anode electrodes for the direct methanol fuel cell. Catalysts were produced as aerosol nanoparticles in a spray-flame reactor and deposited directly as a thin layer on the gas diffusion layer. The as-prepared catalyst wa......Ru1/Vulcan carbon. The kinetics of methanol oxidation on the mixed phase catalyst was also explored by electrochemical impedance spectroscopy. (c) 2005 The Electrochemical Society.......A spray-flame aerosol catalyzation technique was studied for producing Pt-Ru anode electrodes for the direct methanol fuel cell. Catalysts were produced as aerosol nanoparticles in a spray-flame reactor and deposited directly as a thin layer on the gas diffusion layer. The as-prepared catalyst...... was found to be a mixture of nanocrystalline, mostly unalloyed Pt and an amorphous phase mostly of Ru and to a lesser extent of Pt oxides on top of the crystalline phase. The flame-produced Pt1Ru1 demonstrated similar onset potential but similar to 60% higher activity compared to commercially available Pt1...

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.

Direct sorbitol proton exchange membrane fuel cell using moderate catalyst loadings

International Nuclear Information System (INIS)

Oyarce, Alejandro; Gonzalez, Carlos; Lima, Raquel Bohn; Lindström, Rakel Wreland; Lagergren, Carina; Lindbergh, Göran

2014-01-01

Highlights: •The performance of a direct sorbitol fuel cell was evaluated at different temperatures. •The performance was compared to the performance of a direct glucose fuel cell. •The mass specific peak power density of the direct sorbitol fuel cell was 3.6 mW mg −1 totalcatalystloading at 80 °C. •Both sorbitol and glucose fuel cell suffer from deactivation. -- Abstract: Recent progress in biomass hydrolysis has made it interesting to study the use of sorbitol for electricity generation. In this study, sorbitol and glucose are used as fuels in proton exchange membrane fuel cells having 0.9 mg cm −2 PtRu/C at the anode and 0.3 mg cm −2 Pt/C at the cathode. The sorbitol oxidation was found to have slower kinetics than glucose oxidation. However, at low temperatures the direct sorbitol fuel cell shows higher performance than the direct glucose fuel cell, attributed to a lower degree of catalyst poisoning. The performance of both fuel cells is considerably improved at higher temperatures. High temperatures lower the poisoning, allowing the direct glucose fuel cell to reach a higher performance than the direct sorbitol fuel cell. The mass specific peak power densities of the direct sorbitol and direct glucose fuel cells at 65 °C was 3.2 mW mg −1 catalyst and 3.5 mW mg −1 catalyst , respectively. Both of these values are one order of magnitude larger than mass specific peak power densities of earlier reported direct glucose fuel cells using proton exchange membranes. Furthermore, both the fuel cells showed a considerably decrease in performance with time, which is partially attributed to sorbitol and glucose crossover poisoning the Pt/C cathode

Search Directions for Direct H2O2 Synthesis Catalysts Starting from Au-12 Nanoclusters

DEFF Research Database (Denmark)

Grabow, Lars; Larsen, Britt Hvolbæk; Falsig, Hanne

2012-01-01

that the rate of H2O2 and H2O formation can be determined from a single descriptor, namely, the binding energy of oxygen (E-O). Our model predicts the search direction starting from an Au-12 nanocluster for an optimal catalyst in terms of activity and selectivity for direct H2O2 synthesis. Taking also stability......We present density functional theory calculations on the direct synthesis of H2O2 from H-2 and O-2 over an Au-12 corner model of a gold nanoparticle. We first show a simple route for the direct formation of H2O2 over a gold nanocatalyst, by studying the energetics of 20 possible elementary...... reactions involved in the oxidation of H-2 by O-2. The unwanted side reaction to H2O is also considered. Next we evaluate the degree of catalyst control and address the factors controlling the activity and the selectivity. By combining well-known energy scaling relations with microkinetic modeling, we show...

Electrical enhancement of direct methanol fuel cells by metal-plasma ion implantation Pt-Ru/C multilayer catalysts.

Science.gov (United States)

Weng, Ko-Wei; Chen, Yung-Lin; Chen, Ya-Chi; Lin, Tai-Nan

2009-02-01

Direct methanol fuel cells (DMFC) have been widely studied owing to their simple cell configuration, high volume energy density, short start-up time, high operational reliability and other favorable characteristics. However, major limitations include high production cost, poisoning of the catalyst and methanol crossover. This study adopts a simple technique for preparing Pt-Ru/C multilayer catalysts, including magnetron sputtering (MS) and metal-plasma ion implantation (MPII). The Pt catalysts were sputtered onto the gas diffusion layer (GDL), followed by the implantation of Ru catalysts using MPII (at an accelerating voltage of 20 kV and an implantation dose of 1 x 10(16) ions/cm2). Pt-Ru is repeatedly processed to prepare Pt-Ru/C multilayer catalysts. The catalyst film structure and microstructure were analyzed by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electronic microscopy (SEM), respectively. The cell performance was tested using a potential stat/galvano-stat. The results reveal that the membrane electrode assembly (MEA) of four multilayer structures enhances the cell performance of DMFC. The measured power density is 2.2 mW/cm2 at a methanol concentration of 2 M, with an OCV of 0.493 V.

Silver-palladium catalysts for the direct synthesis of hydrogen peroxide

Science.gov (United States)

Khan, Zainab; Dummer, Nicholas F.; Edwards, Jennifer K.

2017-11-01

A series of bimetallic silver-palladium catalysts supported on titania were prepared by wet impregnation and assessed for the direct synthesis of hydrogen peroxide, and its subsequent side reactions. The addition of silver to a palladium catalyst was found to significantly decrease hydrogen peroxide productivity and hydrogenation, but crucially increase the rate of decomposition. The decomposition product, which is predominantly hydroxyl radicals, can be used to decrease bacterial colonies. The interaction between silver and palladium was characterized using scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy (XPS) and temperature programmed reduction (TPR). The results of the TPR and XPS indicated the formation of a silver-palladium alloy. The optimal 1% Ag-4% Pd/TiO2 bimetallic catalyst was able to produce approximately 200 ppm of H2O2 in 30 min. The findings demonstrate that AgPd/TiO2 catalysts are active for the synthesis of hydrogen peroxide and its subsequent decomposition to reactive oxygen species. The catalysts are promising for use in wastewater treatment as they combine the disinfectant properties of silver, hydrogen peroxide production and subsequent decomposition. This article is part of a discussion meeting issue 'Providing sustainable catalytic solutions for a rapidly changing world'.

Direct hydrothermal liquefaction of undried macroalgae Enteromorpha prolifera using acid catalysts

International Nuclear Information System (INIS)

Yang, Wenchao; Li, Xianguo; Liu, Shishi; Feng, Lijuan

2014-01-01

Highlights: • Bio-oil from liquefaction of wet E. prolifera was as feasible as dry powder. • Adding acid catalysts could improve the flow property of bio-oil. • Alkenes in the bio-oil converted to ketones in the presence of acid catalysts. • Content of 5-methyl furfural increased in the bio-oil obtained with acid catalysts. • Esters were formed in the bio-oil when adding sulfuric acid as a catalyst. - Abstract: Direct liquefaction of macroalgae Enteromorpha prolifera without predrying treatment was performed in a batch reactor. Effects of temperature, reaction time, biomass-to-water ratio and acid catalysts (sulfuric acid and acetic acid) on liquefaction products were investigated. Raw material and liquefaction products were analyzed by elemental analysis, Fourier transform infrared (FT-IR) and gas chromatography–mass spectrometry (GC–MS). Results showed that liquefaction at 290 °C for 20 min with 1:3 biomass-to-water ratio produced the highest bio-oil yield of 28.4 wt%, and high heating value (HHV) was 29.5 MJ/kg. Main components of bio-oil were fatty acids, ketones, alkenes and 5-methyl furfural, and main components of water soluble organics (WSOs) were pyridines, carboxylic acids and glycerol. In the bio-oil obtained with acid catalysts, content of ketones significantly increased while alkenes disappeared. Content of 5-methyl furfural also increased. Flow property of bio-oils was improved in the presence of acid catalysts. Moreover, esters were formed when adding sulfuric acid

Activity of platinum/carbon and palladium/carbon catalysts promoted by Ni2 P in direct ethanol fuel cells.

Science.gov (United States)

Li, Guoqiang; Feng, Ligang; Chang, Jinfa; Wickman, Björn; Grönbeck, Henrik; Liu, Changpeng; Xing, Wei

2014-12-01

Ethanol is an alternative fuel for direct alcohol fuel cells, in which the electrode materials are commonly based on Pt or Pd. Owing to the excellent promotion effect of Ni2 P that was found in methanol oxidation, we extended the catalyst system of Pt or Pd modified by Ni2 P in direct ethanol fuel cells. The Ni2 P-promoted catalysts were compared to commercial catalysts as well as to reference catalysts promoted with only Ni or only P. Among the studied catalysts, Pt/C and Pd/C modified by Ni2 P (30 wt %) showed both the highest activity and stability. Upon integration into the anode of a homemade direct ethanol fuel cell, the Pt-Ni2 P/C-30 % catalyst showed a maximum power density of 21 mW cm(-2) , which is approximately two times higher than that of a commercial Pt/C catalyst. The Pd-Ni2 P/C-30 % catalyst exhibited a maximum power density of 90 mW cm(-2) . This is approximately 1.5 times higher than that of a commercial Pd/C catalyst. The discharge stability on both two catalysts was also greatly improved over a 12 h discharge operation. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Directed plant cell-wall accumulation of iron: embedding co-catalyst for efficient biomass conversion

Science.gov (United States)

Chien-Yuan Lin; Joseph E. Jakes; Bryon S. Donohoe; Peter N. Ciesielski; Haibing Yang; Sophie-Charlotte Gleber; Stefan Vogt; Shi-You Ding; Wendy A. Peer; Angus S. Murphy; Maureen C. McCann; Michael E. Himmel; Melvin P. Tucker; Hui Wei

2016-01-01

Background: Plant lignocellulosic biomass is an abundant, renewable feedstock for the production of biobased fuels and chemicals. Previously, we showed that iron can act as a co-catalyst to improve the deconstruction of lignocellulosic biomass. However, directly adding iron catalysts into biomass prior to pretreatment is diffusion limited,...

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.

Palladium-alloy catalysts as ethanol tolerant cathodes for direct alcohol fuel cell applications

Energy Technology Data Exchange (ETDEWEB)

Savadogo, O. [Ecole Polytechnique de Montreal, Montreal, PQ (Canada). Laboratoire de nouveaux materiaux pour l' energie et l' electrochimie; Varela, F.J.R. [Centro de Investigacion y de Estudios Avanzados, Coahuila (Mexico). Unidad Saltillo

2008-07-01

Recent studies have demonstrated that electroactive palladium (Pd) and Pd-alloy catalysts prepared using a sputtering technique possess a similar degree of activity as platinum (Pt) electrodes. This study demonstrated that Pd and Pd-alloys show a high degree of tolerance to ethanol during oxygen reduction reaction (ORR) processes. The onset potential of the ORR process in the presence of 0.5M of ethanol decreased by only 33 mV and 18 mV on Pd and Pd-cobalt (Co) catalysts. Linear sweep voltammetry experiments showed that no peak current density caused by the electro-oxidation of ethanol was observed in the Pd-based catalysts. The selective behaviour of the Pd and Pd-Co catalysts was attributed to a slow rate of adsorption of the ethanol as well as the presence of reaction intermediates on the catalytic surface. Results suggested that the Pd and Pd-Co catalysts are suitable candidates for direct alcohol fuel cell applications. 10 refs., 2 figs.

Co, Fe and Ni catalysts supported on coke for direct coal liquefaction

International Nuclear Information System (INIS)

Jimenez, Jose A; Villalba, Oscar A; Rodriguez, Luis I; Hernandez, Orlando; Agamez, Yasmin Y; Dias Jose de Jesus

2008-01-01

Transition metal catalysts supported on coke were prepared by impregnation with a solution of complex of metal-thiourea, that is produced from salt precursors of cobalt chloride, Nickel chloride or iron sulfate and ammonium. sulphide formation on the support surface was generated by decomposition of the metal complex. The catalysts obtained were used in direct coal liquefaction of a medium volatile bituminous coal (Yerbabuena N 1) from Cundinamarca using a 250 Ml, Parr reactor at 723 K and a hydrogen-donor solvent. The catalytic results show, for all samples, both a good coal conversion and an enhancement of the yield of oils, this indicates that the proposed preparation method of catalyst is effective and that eventually the H 2 S sulphidation conventional process could be replaced

Investigation of the Performance of Aucore-Pdshell/C as the Anode Catalyst of Direct Borohydride-Hydrogen Peroxide Fuel Cell

Directory of Open Access Journals (Sweden)

Hong Wang

2011-01-01

Full Text Available The carbon-supported bimetallic Au-Pd catalyst with core-shell structure is prepared by successive reduction method. The core-shell structure, surface morphology, and electrochemical performances of the catalysts are characterized by X-ray diffraction (XRD, transmission electron microscopy (TEM, ultraviolet-visible absorption spectrometry, linear sweep voltammetry, and chronopotentiometry. The results show that the Au-Pd/C catalyst with core-shell structure exhibits much higher catalytic activity for the direct oxidation of NaBH4 than pure Au/C catalyst. A direct borohydride-hydrogen peroxide fuel cell, in which the Au-Pd/C with core-shell structure is used as the anode catalyst and the Au/C as the cathode catalyst, shows as high as 68.215 mW cm−2 power density.

Ni2P Makes Application of the PtRu Catalyst Much Stronger in Direct Methanol Fuel Cells.

Science.gov (United States)

Chang, Jinfa; Feng, Ligang; Liu, Changpeng; Xing, Wei

2015-10-12

PtRu is regarded as the best catalyst for direct methanol fuel cells, but the performance decay resulting from the loss of Ru seriously hinders commercial applications. Herein, we demonstrated that the presence of Ni2 P largely reduces Ru loss, which thus makes the application of PtRu much stronger in direct methanol fuel cells. Outstanding catalytic activity and stability were observed by cyclic voltammetry. Upon integrating the catalyst material into a practical direct methanol fuel cell, the highest maximum power density was achieved on the PtRu-Ni2P/C catalyst among the reference catalysts at different temperatures. A maximum power density of 69.9 mW cm(-2) at 30 °C was obtained on PtRu-Ni2P/C, which is even higher than the power density of the state-of-the-art commercial PtRu catalyst at 70 °C (63.1 mW cm(-2)). Moreover, decay in the performance resulting from Ru loss was greatly reduced owing to the presence of Ni2 P, which is indicative of very promising applications. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Methanol electro-oxidation and direct methanol fuel cell using Pt/Rh and Pt/Ru/Rh alloy catalysts

International Nuclear Information System (INIS)

Choi, Jong-Ho; Park, Kyung-Won; Park, In-Su; Nam, Woo-Hyun; Sung, Yung-Eun

2004-01-01

Pt-based binary or ternary catalysts containing Rh for use as anodes in direct methanol fuel cells (DMFC) were synthesized by borohydride reduction method combined with freeze-drying. The resulting catalysts had a specific surface area of approximately 65-75 m 2 /g. X-ray diffraction (XRD) patterns indicated that the catalysts were well alloyed and the average size of alloy catalysts was confirmed by transmission electron microscopy (TEM). The Pt/Rh (2:1) and Pt/Ru/Rh (5:4:1) alloy catalysts showed better catalytic activities for methanol electro-oxidation than Pt or Pt/Ru (1:1), respectively

Direct dimethyl-ether (DME) synthesis by spatial patterned catalyst arrangement. A modeling and simulation study

Energy Technology Data Exchange (ETDEWEB)

McBride, K.; Turek, T.; Guettel, R. [Clausthal Univ. of Technology (Germany). Inst. of Chemical Process Engineering

2011-07-01

The effect of spatially patterned catalyst beds was investigated for direct DME synthesis from synthesis gas as an example. A layered arrangement of methanol synthesis and dehydration catalyst was chosen and studied by numerical simulation under typical operating conditions for single-step DME synthesis. It was revealed that catalyst layers significantly influence the DME productivity. With an increasing number of layers from 2 to 40, an increase in DME productivity was observed approaching the performance of a physical catalyst mixture for an infinite number of layers. The results prove that a physical mixture of methanol synthesis and dehydration catalyst achieves the highest DME productivity under operating conditions chosen in this study. This can be explained by the higher average methanol concentration for the layered catalyst arrangement and thus stronger equilibrium constraints for the methanol synthesis reaction. Essentially, the layered catalyst arrangement is comparable to a cascade model of the two-step process, which is less efficient in terms of DME yield than the single-step process. However, since a significant effect was found, the layered catalyst arrangement could be beneficial for other reaction systems. (orig.)

Synthesis and characterization of Cu-MFI catalyst for the direct medium temperature range NO decomposition

Directory of Open Access Journals (Sweden)

Valkaj Karolina Maduna

2016-03-01

Full Text Available In this study the physico-chemical and catalytic properties of copper bearing MFI zeolites (Cu-MFI with different Si/Al and Si/Cu ratios were investigated. Two different methods for incorporation of metal ions into the zeolite framework were used: the ion exchange from the solution of copper acetate and the direct hydrothermal synthesis. Direct synthesis of a zeolite in the presence of copper-phosphate complexes was expected to generate more active copper species necessary for the desired reaction than the conventional ion exchange method. Direct decomposition of NO was used as a model reaction, because this reaction still offers a very attractive approach to NOX removal. The catalytic properties of zeolite samples were studied using techniques, such as XRD, SEM, EPR and nitrogen adsorption/desorption measurements at 77 K. Results of the kinetic investigation revealed that both methods are applicable for the preparation of the catalysts with active sites capable of catalyzing the NO decomposition. It was found out that Cu-MFI zeolites obtained through direct synthesis are promising catalysts for NO decomposition, especially at lower reaction temperatures. The efficiency of the catalysts prepared by both methods is compared and discussed.

Direct NO decomposition over conventional and mesoporous Cu-ZSM-5 and Cu-ZSM-11 catalysts

DEFF Research Database (Denmark)

Kustova, Marina; Rasmussen, Søren Birk; Kustov, Arkadii

2006-01-01

Conventional Cu-ZSM-5 has for many years been recognized as a unique catalyst for direct NO decomposition. Zeolite-based catalysts have a crystallographically well-defined microporous structure. In such microporous catalysts, the creation and accessibility of the active sites is often influenced...... that ZSM-11 has only straight microporous channels, while ZSNI-5 has both straight and sinusoidal channels. Apparently, there is a preferential formation of active sites and/or improved accessibility in the straight channels compared to the sinusoidal channels, which make the ZSM-11 material a better...

Co-catalytic effect of Ni in the methanol electro-oxidation on Pt-Ru/C catalyst for direct methanol fuel cell

International Nuclear Information System (INIS)

Wang, Z.B.; Yin, G.P.; Zhang, J.; Sun, Y.C.; Shi, P.F.

2006-01-01

This research is aimed to improve the utilization and activity of anodic catalysts, thus to lower the contents of noble metals loading in anodes for methanol electro-oxidation. The direct methanol fuel cell anodic catalysts, Pt-Ru-Ni/C and Pt-Ru/C, were prepared by chemical reduction method. Their performances were tested by using a glassy carbon working electrode through cyclic voltammetric curves, chronoamperometric curves and half-cell measurement in a solution of 0.5 mol/L CH 3 OH and 0.5 mol/L H 2 SO 4 . The composition of the Pt-Ru-Ni and Pt-Ru surface particles were determined by EDAX analysis. The particle size and lattice parameter of the catalysts were determined by means of X-ray diffraction (XRD). XRD analysis showed that both of the catalysts exhibited face-centered cubic structures and had smaller lattice parameters than Pt-alone catalyst. Their sizes are small, about 4.5 nm. No significant differences in the methanol electro-oxidation on both electrodes were found by using cyclic voltammetry, especially regarding the onset potential for methanol electro-oxidation. The electrochemically active-specific areas of the Pt-Ru-Ni/C and Pt-Ru/C catalysts are almost the same. But, the catalytic activity of the Pt-Ru-Ni/C catalyst is higher for methanol electro-oxidation than that of the Pt-Ru/C catalyst. Its tolerance performance to CO formed as one of the intermediates of methanol electro-oxidation is better than that of the Pt-Ru/C catalyst

A durable PtRu/C catalyst with a thin protective layer for direct methanol fuel cells.

Science.gov (United States)

Shimazaki, Yuzuru; Hayasaka, Sho; Koyama, Tsubasa; Nagao, Daisuke; Kobayashi, Yoshio; Konno, Mikio

2010-11-15

A methanol oxidation catalyst with improved durability in acidic environments is reported. The catalyst consists of PtRu alloy nanoparticles on a carbon support that were stabilized with a silane-coupling agent. The catalyst was prepared by reducing ions of Pt and Ru in the presence of a carbon support and the silane-coupling agent. The careful choice of preparatory conditions such as the concentration of the silane-coupling agent and solution pH resulted in the preparation of catalyst in which the PtRu nanoparticles were dispersively adsorbed onto the carbon support. The catalytic activity was similar to that of a commercial catalyst and was unchanged after immersion in sulfuric acid solution for 1000 h, suggesting the high durability of the PtRu catalyst for the anode of direct methanol fuel cells. Copyright © 2010 Elsevier Inc. All rights reserved.

Vitrification of nanotoxic waste (Ru) from the production of nano-catalysts for direct ethanol fuel cells

International Nuclear Information System (INIS)

Silva, A.C.; Julio-Junior, O.; Mello-Castanho, S.R.H.

2010-01-01

Nanostructured catalysts have been developed for ethanol directly use in fuel cells, which due to the economic advantages that should have widespread use in the near future. The catalysts for these devices using nano-structured metal are based, where the toxic nature and environmental risks presented by these metals are largely enhanced by nano-dispersion. Thus, the production of nano-catalysts are potentially generating highly hazardous waste for public health and the environment. This study presents the treatment and inertization of ruthenium (Ru) nanoparticles waste containing by the vitrification technique and consequent attainment of silicate glasses for potential commercial use. Compositions were prepared containing up to about 20 wt % of nano-waste by changing the basic composition of glass soda-lime-borosilicate. After the fusion, at a temperature of 1100 deg C, the glasses were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and Infra-red in the Fourier transform (FT-IR) techniques. The chemical stability was evaluated by hydrolytic attack test. The glass containing 20 wt % of nano-residue showed a high chemical stability, similar to a usual soda-lime glass. (author)

Use of phyllosilicates in electrochemical devices: possible use of sepiolite as a support of catalysts in direct alcohol fuel cells (DAFC)

International Nuclear Information System (INIS)

Parra-Silva, J.; Silva, A.C.; Mello-Castanho, S.R.H.; Cerpa, A.

2014-01-01

Direct alcohol Fuel cells (DAFC) are interesting to use Brazil for reasons of fuel logistics and availability. The catalysts used in these devices to promote the oxidation of alcohol at the anode need to be fixed on a substrate which must provide high specific surface area, porosity, chemical and thermal resistance, this target can be achieved with the characteristics sepiolite. This paper proposes sepiolite as catalyst support for DAFC. Sepiolite is a phyllosilicate with double layered tetrahedral silicon cells and fibrillar structure. Catalysts (Pt / Sb / Sn) were prepared by cation substitution method and tested by cyclic voltammetry. Techniques as XRD and FT-IR were also used for characterizing materials. Was obtained up to 35 mA / g (Pt) peak current (redox ethanol) indicating the possibility of sepiolite technology development to use un proposed purpose. (author)

Performance of an Active Micro Direct Methanol Fuel Cell Using Reduced Catalyst Loading MEAs

Directory of Open Access Journals (Sweden)

D.S. Falcão

2017-10-01

Full Text Available The micro direct methanol fuel cell (MicroDMFC is an emergent technology due to its special interest for portable applications. This work presents the results of a set of experiments conducted at room temperature using an active metallic MicroDMFC with an active area of 2.25 cm2. The MicroDMFC uses available commercial materials with low platinum content in order to reduce the overall fuel cell cost. The main goal of this work is to provide useful information to easily design an active MicroDMFC with a good performance recurring to cheaper commercial Membrane Electrode Assemblies MEAs. A performance/cost analysis for each MEA tested is provided. The maximum power output obtained was 18.1 mW/cm2 for a hot-pressed MEA with materials purchased from Quintech with very low catalyst loading (3 mg/cm2 Pt–Ru at anode side and 0.5 mg/cm2 PtB at the cathode side costing around 15 euros. Similar power values are reported in literature for the same type of micro fuel cells working at higher operating temperatures and substantially higher cathode catalyst loadings. Experimental studies using metallic active micro direct methanol fuel cells operating at room temperature are very scarce. The results presented in this work are, therefore, very useful for the scientific community.

Fuel Cell Stations Automate Processes, Catalyst Testing

Science.gov (United States)

2010-01-01

Glenn Research Center looks for ways to improve fuel cells, which are an important source of power for space missions, as well as the equipment used to test fuel cells. With Small Business Innovation Research (SBIR) awards from Glenn, Lynntech Inc., of College Station, Texas, addressed a major limitation of fuel cell testing equipment. Five years later, the company obtained a patent and provided the equipment to the commercial world. Now offered through TesSol Inc., of Battle Ground, Washington, the technology is used for fuel cell work, catalyst testing, sensor testing, gas blending, and other applications. It can be found at universities, national laboratories, and businesses around the world.

Effect of the Pd/MWCNTs anode catalysts preparation methods on their morphology and activity in a direct formic acid fuel cell

Energy Technology Data Exchange (ETDEWEB)

Lesiak, B., E-mail: blesiak-orlowska@ichf.edu.pl [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warszawa (Poland); Mazurkiewicz, M.; Malolepszy, A. [Faculty of Chemical and Process Engineering, Warsaw University of Technology, Waryńskiego 1, 00-645 Warszawa (Poland); Stobinski, L. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warszawa (Poland); Faculty of Chemical and Process Engineering, Warsaw University of Technology, Waryńskiego 1, 00-645 Warszawa (Poland); Mierzwa, B.; Mikolajczuk-Zychora, A.; Juchniewicz, K.; Borodzinski, A. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warszawa (Poland); Zemek, J.; Jiricek, P. [Institute of Physics, Academy of Sciences of the Czech Republic, 162-53 Prague 6, Cukrovarnicka 10 (Czech Republic)

2016-11-30

Highlights: • Catalysts properties studied by XRD, STEM, XPS methods. • Differences in Pd particle size, content of Pd, functional groups, PdC{sub x.}. • Catalytic activity studied in a Direct Formic Acid Fuel Cell. • Highest activity–catalyst prepared using a strong reducing agent (NaBH{sub 4}). - Abstract: Impact of Pd/MWCNTs catalysts preparation method on the catalysts morphology and activity in a formic acid electrooxidation reaction was investigated. Three reduction methods of Pd precursor involving reduction in a high pressure microwave reactor (Pd1), reduction with NaBH{sub 4} (Pd2) and microwave-assisted polyol method (Pd3) were used in this paper. Crystallites size and morphology were studied using the scanning transmission electron microscopy (STEM), X-ray diffraction (XRD), whereas elemental composition, Pd chemical state and functional groups content by the X-ray photoelectron spectroscopy (XPS). The prepared catalysts were tested in a direct formic acid fuel cell (DFAFC) as an anode material. The catalytic activity was correlated with a mean fraction of the total Pd atoms exposed at the surface (FE). The value of FE was calculated from the crystallites size distribution determined by the STEM measurements. Non-linear dependence of a current density versus FE, approaching the maximum at FE≈0.25 suggests that the catalytic process proceeded at Pd nanocrystallites faces, with inactive edges and corners. Pd2 catalyst exhibited highest activity due to its smallest Pd crystallites (3.2 nm), however the absence of Pd crystallites aggregation and low content of carbon in PdC{sub x} phase, i.e. x = 4 at.% may also affect the observed.

Effect of the Pd/MWCNTs anode catalysts preparation methods on their morphology and activity in a direct formic acid fuel cell

International Nuclear Information System (INIS)

Lesiak, B.; Mazurkiewicz, M.; Malolepszy, A.; Stobinski, L.; Mierzwa, B.; Mikolajczuk-Zychora, A.; Juchniewicz, K.; Borodzinski, A.; Zemek, J.; Jiricek, P.

2016-01-01

Highlights: • Catalysts properties studied by XRD, STEM, XPS methods. • Differences in Pd particle size, content of Pd, functional groups, PdC x. . • Catalytic activity studied in a Direct Formic Acid Fuel Cell. • Highest activity–catalyst prepared using a strong reducing agent (NaBH 4 ). - Abstract: Impact of Pd/MWCNTs catalysts preparation method on the catalysts morphology and activity in a formic acid electrooxidation reaction was investigated. Three reduction methods of Pd precursor involving reduction in a high pressure microwave reactor (Pd1), reduction with NaBH 4 (Pd2) and microwave-assisted polyol method (Pd3) were used in this paper. Crystallites size and morphology were studied using the scanning transmission electron microscopy (STEM), X-ray diffraction (XRD), whereas elemental composition, Pd chemical state and functional groups content by the X-ray photoelectron spectroscopy (XPS). The prepared catalysts were tested in a direct formic acid fuel cell (DFAFC) as an anode material. The catalytic activity was correlated with a mean fraction of the total Pd atoms exposed at the surface (FE). The value of FE was calculated from the crystallites size distribution determined by the STEM measurements. Non-linear dependence of a current density versus FE, approaching the maximum at FE≈0.25 suggests that the catalytic process proceeded at Pd nanocrystallites faces, with inactive edges and corners. Pd2 catalyst exhibited highest activity due to its smallest Pd crystallites (3.2 nm), however the absence of Pd crystallites aggregation and low content of carbon in PdC x phase, i.e. x = 4 at.% may also affect the observed.

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

Direct conversion of CO2 into liquid fuels with high selectivity over a bifunctional catalyst

Science.gov (United States)

Gao, Peng; Li, Shenggang; Bu, Xianni; Dang, Shanshan; Liu, Ziyu; Wang, Hui; Zhong, Liangshu; Qiu, Minghuang; Yang, Chengguang; Cai, Jun; Wei, Wei; Sun, Yuhan

2017-10-01

Although considerable progress has been made in carbon dioxide (CO2) hydrogenation to various C1 chemicals, it is still a great challenge to synthesize value-added products with two or more carbons, such as gasoline, directly from CO2 because of the extreme inertness of CO2 and a high C-C coupling barrier. Here we present a bifunctional catalyst composed of reducible indium oxides (In2O3) and zeolites that yields a high selectivity to gasoline-range hydrocarbons (78.6%) with a very low methane selectivity (1%). The oxygen vacancies on the In2O3 surfaces activate CO2 and hydrogen to form methanol, and C-C coupling subsequently occurs inside zeolite pores to produce gasoline-range hydrocarbons with a high octane number. The proximity of these two components plays a crucial role in suppressing the undesired reverse water gas shift reaction and giving a high selectivity for gasoline-range hydrocarbons. Moreover, the pellet catalyst exhibits a much better performance during an industry-relevant test, which suggests promising prospects for industrial applications.

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.

High Performance and Cost-Effective Direct Methanol Fuel Cells: Fe-N-C Methanol-Tolerant Oxygen Reduction Reaction Catalysts.

Science.gov (United States)

Sebastián, David; Serov, Alexey; Artyushkova, Kateryna; Gordon, Jonathan; Atanassov, Plamen; Aricò, Antonino S; Baglio, Vincenzo

2016-08-09

Direct methanol fuel cells (DMFCs) offer great advantages for the supply of power with high efficiency and large energy density. The search for a cost-effective, active, stable and methanol-tolerant catalyst for the oxygen reduction reaction (ORR) is still a great challenge. In this work, platinum group metal-free (PGM-free) catalysts based on Fe-N-C are investigated in acidic medium. Post-treatment of the catalyst improves the ORR activity compared with previously published PGM-free formulations and shows an excellent tolerance to the presence of methanol. The feasibility for application in DMFC under a wide range of operating conditions is demonstrated, with a maximum power density of approximately 50 mW cm(-2) and a negligible methanol crossover effect on the performance. A review of the most recent PGM-free cathode formulations for DMFC indicates that this formulation leads to the highest performance at a low membrane-electrode assembly (MEA) cost. Moreover, a 100 h durability test in DMFC shows suitable applicability, with a similar performance-time behavior compared to common MEAs based on Pt cathodes. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Impact of anode catalyst layer porosity on the performance of a direct formic acid fuel cell

International Nuclear Information System (INIS)

Bauskar, Akshay S.; Rice, Cynthia A.

2012-01-01

Highlights: ► Lithium carbonate is used as a pore-former to increase porosity of anode catalyst layer. ► Maximum power density increased by 25%. ► Onset potential for formic acid electro-oxidation reduced by 30 mV for anode catalyst layer with 17.5 wt% pore-former. ► Electrochemical impedance spectra confirm increased formic acid concentration inside the anode catalyst layer pores. - Abstract: Direct formic acid fuel cells (DFAFCs) have attracted much attention in the last few years for portable electronic devices, due to their potential of being high efficiency power sources. They have the potential to replace the state-of-the-art batteries in cell phones, PDAs, and laptop computers if their power density and durability can be improved. In the present investigation, the influence of increased anode catalyst layer porosity on DFAFC power density performance is studied. Lithium carbonate (Li 2 CO 3 ) was used as a pore-former in this study because of its facile and complete removal after catalyst layer fabrication. The anode catalyst layers presented herein contained unsupported Pt/Ru catalyst and Li 2 CO 3 (in the range of 0–50 wt%) bound with proton conducting ionomer. Higher DFAFC performance is obtained because of the increased porosity within the anode catalyst layer through enhanced reactant and product mass transport. The maximum power density of DFAFC increased by 25% when pore-former was added to the anode catalyst ink. The formic acid onset potential for the anode catalyst layer with 17.5 wt% pore-former was reduced by 30 mV. A constant phase element based equivalent-circuit model was used to investigate anode impedance spectra. Fitted values for the anode impedance spectra confirm the improvement in performance due to an increase in formic acid concentration inside the anode catalyst layer pores along with efficient transport of reactants and products.

Direct Fabrication of Carbon Nanotubes STM Tips by Liquid Catalyst-Assisted Microwave Plasma-Enhanced Chemical Vapor Deposition

Directory of Open Access Journals (Sweden)

Fa-Kuei Tung

2009-01-01

Full Text Available Direct and facile method to make carbon nanotube (CNT tips for scanning tunneling microscopy (STM is presented. Cobalt (Co particles, as catalysts, are electrochemically deposited on the apex of tungsten (W STM tip for CNT growth. It is found that the quantity of Co particles is well controlled by applied DC voltage, concentration of catalyst solution, and deposition time. Using optimum growth condition, CNTs are successfully synthesized on the tip apex by catalyst-assisted microwave-enhanced chemical vapor deposition (CA-MPECVD. A HOPG surface is clearly observed at an atomic scale using the present CNT-STM tip.

Effect of the nanosized TiO2 particles in Pd/C catalysts as cathode materials in direct methanol fuel cells.

Science.gov (United States)

Choi, Mahnsoo; Han, Choonsoo; Kim, In-Tae; Lee, Ji-Jung; Lee, Hong-Ki; Shim, Joongpyo

2011-07-01

Pd-TiO2/C catalysts were prepared by impregnating titanium dioxide (TiO2) on carbon-supported Pd (Pd/C) for use as the catalyst for the oxygen reduction reaction (ORR) in direct methanol fuel cells (DMFCs). Transmission electron microscope (TEM), scanning electron microscope (SEM) and X-ray diffraction (XRD) analyses were carried to confirm the distribution, morphology and structure of Pd and TiO2 on the carbon support. In fuel cell test, we confirmed that the addition of TiO2 nanoparticles make the improved catalytic activity of oxygen reduction. The electrochemical characterization of the Pd-TiO2/C catalyst for the ORR was carried out by cyclic voltammetry (CV) in the voltage window of 0.04 V to 1.2 V with scan rate of 25 mV/s. With the increase in the crystallite size of TiO2, the peak potential for OH(ads) desorption on the surface of Pd particle shifted to higher potential. This implies that TiO2 might affect the adsorption and desorption of oxygen molecules on Pd catalyst. The performance of Pd-TiO2/C as a cathode material was found to be similar to or better performance than that of Pt/C.

On the Preparation and Testing of Fuel Cell Catalysts Using the Thin Film Rotating Disk Electrode Method.

Science.gov (United States)

Inaba, Masanori; Quinson, Jonathan; Bucher, Jan Rudolf; Arenz, Matthias

2018-03-16

We present a step-by-step tutorial to prepare proton exchange membrane fuel cell (PEMFC) catalysts, consisting of Pt nanoparticles (NPs) supported on a high surface area carbon, and to test their performance in thin film rotating disk electrode (TF-RDE) measurements. The TF-RDE methodology is widely used for catalyst screening; nevertheless, the measured performance sometimes considerably differs among research groups. These uncertainties impede the advancement of new catalyst materials and, consequently, several authors discussed possible best practice methods and the importance of benchmarking. The visual tutorial highlights possible pitfalls in the TF-RDE testing of Pt/C catalysts. A synthesis and testing protocol to assess standard Pt/C catalysts is introduced that can be used together with polycrystalline Pt disks as benchmark catalysts. In particular, this study highlights how the properties of the catalyst film on the glassy carbon (GC) electrode influence the measured performance in TF-RDE testing. To obtain thin, homogeneous catalyst films, not only the catalyst preparation, but also the ink deposition and drying procedures are essential. It is demonstrated that an adjustment of the ink's pH might be necessary, and how simple control measurements can be used to check film quality. Once reproducible TF-RDE measurements are obtained, determining the Pt loading on the catalyst support (expressed as Pt wt%) and the electrochemical surface area is necessary to normalize the determined reaction rates to either surface area or Pt mass. For the surface area determination, so-called CO stripping, or the determination of the hydrogen underpotential deposition (Hupd) charge, are standard. For the determination of the Pt loading, a straightforward and cheap procedure using digestion in aqua regia with subsequent conversion of Pt(IV) to Pt(II) and UV-vis measurements is introduced.

EFFLUENT TREATMENT FACILITY PEROXIDE DESTRUCTION CATALYST TESTING

International Nuclear Information System (INIS)

HALGREN DL

2008-01-01

The 200 Area Effluent Treatment Facility (ETF) main treatment train includes the peroxide destruction module (PDM) where the hydrogen peroxide residual from the upstream ultraviolet light/hydrogen peroxide oxidation unit is destroyed. Removal of the residual peroxide is necessary to protect downstream membranes from the strong oxidizer. The main component of the PDM is two reaction vessels utilizing granular activated carbon (GAC) as the reaction media. The PDM experienced a number of operability problems, including frequent plugging, and has not been utilized since the ETF changed to groundwater as the predominant feed. The unit seemed to be underperforming in regards to peroxide removal during the early periods of operation as well. It is anticipated that a functional PDM will be required for wastewater from the vitrification plant and other future streams. An alternate media or methodology needs to be identified to replace the GAC in the PDMs. This series of bench scale tests is to develop information to support an engineering study on the options for replacement of the existing GAC method for peroxide destruction at the ETF. A number of different catalysts will be compared as well as other potential methods such as strong reducing agents. The testing should lead to general conclusions on the viability of different catalysts and identify candidates for further study and evaluation

Vibration measurements of automobile catalyst

Science.gov (United States)

Aatola, Seppo

1994-09-01

Vibration of catalyst cell, which is inside the casing of the catalyst, is difficult to measure with usual measuring instrumentation. When catalyst is in use, there is hot exhaust gas flow though the catalyst cell and temperature of the cell is approximately +900 degree(s)C. Therefore non-contact Laser- Doppler-Vibrometer was used to measure vibration velocity of the catalyst cell. The laser beam was directed towards the cell through pipe which was put through and welded to the casing of the catalyst. The outer end of the pipe was screw down with a tempered class to prevent exhaust gas flow from the pipe. The inner end of the pipe was open and few millimeters away from the measuring point. Catalyst was attached to the engine with two ways, rigidly close to the engine and flexible under the engine. The engine was running in test bench under controlled conditions. Vibration measurements were carried out during constant running speeds of the engine. Vibration signals were captured and analyzed with FFT-analyzer. Vibration of catalyst cell was strongest at running speed of 5000 rpm, from 10 to 20 g (1 g equals 9.81 ms-2), when catalyst was attached rigidly close to the engine. At running speed of 3000 rpm, vibration of catalyst cell was from 2 to 3 g in most cases, when catalyst was attached either rigidly or flexible to the engine. It is estimated that in real life, i.e. when catalyst is attached to car with same engine, vibration of catalyst cell at running speed of 5000 rpm is somewhere between 1 and 10 g. At running speed of 3000 rpm, which may be more often used when driving car (car speed approximately 100 kmh-1), vibration of catalyst cell is probably few g's.

Enlarged test catalysts during the hydrogenation of 1,4-butynediol to 1,4-butanediol

Directory of Open Access Journals (Sweden)

Zhaksyntay Kairbekov

2013-09-01

Full Text Available The highly effective catalyzer for butynediol-1;4 hydrogenation was designed and synthesized. Enlarged tests showed that the selectivity on butanediol-1.4 at the hydrogenation of butynediol-1.4 on the alloyed catalyst SKN-39H during 320 h was 84.6 %; that on 18 % higher than for  industrial MNH. The yield of product on the catalyst SKN-39 increases slowly from 3.1 to 7.3 % when on a catalyst MNH – 7.1 to 11.7 % from the initial content of butynediol-1;4. At the hydrogenation of  butynediol on catalyst SKN-39H process efficiency increases in 1.5-2 times and product purity on 2-3 % is higher in comparing with the industrial catalyst MNH. 

Direct conversion of glucose to 5-(hydroxymethyl)furfural in ionic liquids with lanthanide catalysts

DEFF Research Database (Denmark)

Ståhlberg, Tim; Sørensen, Mathilde Grau; Riisager, Anders

2010-01-01

The direct conversion of glucose to 5-(hydroxymethyl)furfural (HMF) in ionic liquids with lanthanide catalysts was examined in search of a possibly more environmentally feasible process not involving chromium. The highest HMF yield was obtained with ytterbium chloride or triflate together...

New Catalysts for Direct Methanol Oxidation Fuel Cells

Energy Technology Data Exchange (ETDEWEB)

Adzic, Radoslav

1998-08-01

A new class of efficient electrocatalytic materials based on platinum - metal oxide systems has been synthetized and characterized by several techniques. Best activity was found with NiWO{sub 4}-, CoWO{sub 4}-, and RuO{sub 2}- sr¡pported platinum catalysts. A very similar activity at room temperature was observed with the electrodes prepared with the catalyst obtained from International Fuel Cells Inc. for the same Pt loading. Surprisingly, the two tungstates per se show a small activity for methanol oxidation without any Pt loading. Synthesis of NiWO{sub 4} and CoWO{sub 4} were carried out by solid-state reactions. FTIR spectroscopy shows that the tungstates contain a certain amount of physically adsorbed water even after heating samples at 200{degrees}C. A direct relationship between the activity for methanol oxidation and the amount of adsorbed water on those oxides has been found. The Ru(0001) single crystal shows a very small activity for CO adsorption and oxidation, in contrast to the behavior of polycrystalline Ru. In situ extended x-ray absorption fine structure spectroscopy (EXAFS) and x-ray absorption near edge spectroscopy (XANES) showed that the OH adsorption on Ru in the Pt-Ru alloy appears to be the limiting step in methanol oxidation. This does not occur for Pt-RuO{SUB 2} electrocatalyst, which explains its advantages over the Pt-Ru alloys. The IFCC electrocatalyst has the properties of the Pt-Ru alloy.

Bifunctional anode catalysts for direct methanol fuel cells

DEFF Research Database (Denmark)

Rossmeisl, Jan; Ferrin, Peter; Tritsaris, Georgios

2012-01-01

Using the binding energy of OH* and CO* on close-packed surfaces as reactivity descriptors, we screen bulk and surface alloy catalysts for methanol electro-oxidation activity. Using these two descriptors, we illustrate that a good methanol electro-oxidation catalyst must have three key properties......: (1) the ability to activate methanol, (2) the ability to activate water, and (3) the ability to react off surface intermediates (such as CO* and OH*). Based on this analysis, an alloy catalyst made up of Cu and Pt should have a synergistic effect facilitating the activity towards methanol electro-oxidation....... Adding Cu to a Pt(111) surface increases the methanol oxidation current by more than a factor of three, supporting our theoretical predictions for improved electrocatalysts....

Comparison of direct and indirect plasma oxidation of NO combined with oxidation by catalyst

DEFF Research Database (Denmark)

Jogi, Indrek; Stamate, Eugen; Irimiea, Cornelia

2015-01-01

of the DBD reactor decreased the long-term efficiency of direct plasma oxidation. At the same time, the efficiency of indirect oxidation increased at elevated reactor temperatures. Additional experiments were carried out to investigate the improvement of indirect oxidation by the introduction of catalyst...

In situ FTIRS study of ethanol electro-oxidation on anode catalysts in direct ethanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Wang, Q.; Sun, G.; Jiang, L.; Zhu, M.; Yan, S.; Wang, G.; Xin, Q. [Chinese Academy of Sciences, Dalian (China). Dalian Inst. of Chemical Physics; Chen, Q.; Li, J.; Jiang, Y.; Sun, S. [Xiamen Univ., Xiamen (China). State Key Lab. for Physical Chemistry of Solid Surfaces

2006-07-01

The low activation of ethanol oxidation at lower temperatures is an obstacle to the development of cost-effective direct ethanol fuel cells (DEFCs). This study used a modified polyol method to prepare carbon-supported platinum (Pt) based catalysts. Carbon supported Pt-based catalysts were fabricated by a modified polyol method and characterized through transmission electron spectroscopy (TEM) and X-ray diffraction (XRD). Results of the study showed that the particles in the Pt/C and PtRu/C and PtSn/C catalysts were distributed on the carbon support uniformly. Diffraction peaks of the Pt shifted positively in the PtRu/C catalysts and negatively in the PtSn/C catalysts. In situ Fourier Transform Infra-red spectroscopy (FTIR) was used to investigate the adsorption and oxidation process of ethanol on the catalysts. Results showed that the electrocatalytic activity of ethanol oxidation on the materials was enhanced. Linear bonded carbon monoxide (CO) was the most strongly absorbed species, and the main products produced by the catalysts were carbon dioxide (CO{sub 2}), acetaldehyde, and acetic acid. Results showed that the PtRu/C catalyst broke the C-C bond more easily than the Pt/C and PtSn/C compounds. However, the results of a linear sweep voltammogram analysis showed that ethanol oxidation of the PtSn/C was enhanced. Bands observed on the compound indicated the formation of acetic acid and acetaldehyde. It was concluded that the enhancement of PtSn/C for ethanol oxidation was due to the formation of acetic acid and acetaldehyde at lower potentials. 4 refs., 1 fig.

Electrochemical characterization of Pt-Ru-Pd catalysts for methanol oxidation reaction in direct methanol fuel cells.

Science.gov (United States)

Choi, M; Han, C; Kim, I T; An, J C; Lee, J J; Lee, H K; Shim, J

2011-01-01

PtRuPd nanoparticles on carbon black were prepared and characterized as electrocatalysts for methanol oxidation reaction in direct methanol fuel cells. Nano-sized Pd (2-4 nm) particles were deposited on Pt/C and PtRu/C (commercial products) by a simple chemical reduction process. The structural and physical information of the PtRuPd/C were confirmed by TEM and XRD, and their electrocatalytic activities were measured by cyclic voltammetry and linear sweep voltammetry. The catalysts containing Pd showed higher electrocatalytic activity for methanol oxidation reaction than the other catalysts. This might be attributed to an increase in the electrochemical surface area of Pt, which is caused by the addition of Pd; this results in increased catalyst utilization.

Evaluation of Pt-Ru-Ni and Pt-Sn-Ni catalysts as anodes in direct ethanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Ribadeneira, Esteban; Hoyos, Bibian A. [Escuela de Procesos y Energia, Facultad de Minas, Universidad Nacional de Colombia, Medellin (Colombia)

2008-05-15

In this study, the electrooxidation of ethanol on carbon supported Pt-Ru-Ni and Pt-Sn-Ni catalysts is electrochemically studied through cyclic voltammetry at 50 C in direct ethanol fuel cells. All electrocatalysts are prepared using the ethylene glycol-reduction process and are chemically characterized by energy-dispersive X-ray analysis (EDX). For fuel cell evaluation, electrodes are prepared by the transfer-decal method. Nickel addition to the anode improves DEFC performance. When Pt{sub 75}Ru{sub 15}Ni{sub 10}/C is used as an anode catalyst, the current density obtained in the fuel cell is greater than that of all other investigated catalysts. Tri-metallic catalytic mixtures have a higher performance relative to bi-metallic catalysts. These results are in agreement with CV results that display greater activity for PtRuNi at higher potentials. (author)

Investigation of a Pt-Fe/C catalyst for oxygen reduction reaction in direct ethanol fuel cells

International Nuclear Information System (INIS)

Castro Luna, A. M.; Bonesi, A.; Triaca, W. E.; Blasi, A. Di; Stassi, A.; Baglio, V.; Antonucci, V.; Arico, A. S.

2010-01-01

Three cathode catalysts (60% Pt/C, 30% Pt/C and 60% Pt-Fe/C), with a particle size of about 2-3 nm, were prepared to investigate the effect of ethanol cross-over on cathode surfaces. All samples were studied in terms of structure and morphology by using X-ray diffraction (XRD) and transmission electron microscopy (TEM) analyses. Their electrocatalytic behavior in terms of oxygen reduction reaction (ORR) was investigated and compared using a rotating disk electrode (RDE). The tolerance of cathode catalysts in the presence of ethanol was evaluated. The Pt-Fe/C catalyst showed both higher ORR activity and tolerance to ethanol cross-over than Pt/C catalysts. Moreover, the more promising catalysts were tested in 5 cm 2 DEFC single cells at 60 and 80 o C. An improvement in single cell performance was observed in the presence of the Pt-Fe catalyst, due to an enhancement in the oxygen reduction kinetics. The maximum power density was 53 mW cm -2 at 2 bar rel. cathode pressure and 80 o C.

Direct synthesis of ethanol from dimethyl ether and syngas over combined H-Mordenite and Cu/ZnO catalysts.

Science.gov (United States)

Li, Xingang; San, Xiaoguang; Zhang, Yi; Ichii, Takashi; Meng, Ming; Tan, Yisheng; Tsubaki, Noritatsu

2010-10-25

Ethanol was directly synthesized from dimethyl ether (DME) and syngas with the combined H-Mordenite and Cu/ZnO catalysts that were separately loaded in a dual-catalyst bed reactor. Methyl acetate (MA) was formed by DME carbonylation over the H-Mordenite catalyst. Thereafter, ethanol and methanol were produced by MA hydrogenation over the Cu/ZnO catalyst. With the reactant gas containing 1.0% DME, the optimized temperature for the reaction was at 493 K to reach 100% conversion. In the products, the yield of methanol and ethanol could reach 46.3% and 42.2%, respectively, with a small amount of MA, ethyl acetate, and CO(2). This process is environmentally friendly as the main byproduct methanol can be recycled to DME by a dehydration reaction. In contrast, for the physically mixed catalysts, the low conversion of DME and high selectivity of methanol were observed.

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

Energy Technology Data Exchange (ETDEWEB)

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

2007-02-15

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

Discovery of fuel cell anode electrocatalysts and dehydrogenation catalysts using combinatorial techniques

Science.gov (United States)

Chan, Benny Chun Wai

A gas diffusion optical screening method was developed for the discovery of catalysts for the electro-oxidation of reformate gas (H2 with 100 ppm CO). The screening cell was designed to accommodate a gas diffusion layer, 715 member catalyst array, and an electrolyte container. Since protons are generated during H2 oxidation, a pH sensitive fluorphore was used to identify active compositions. The cell showed no detectable iR drop across the array and ranked activity of two commercial PtRu and one Pt catalysts. Over 95% of a given catalyst fluoresced at the initial onset potential and a 5 mV difference in onset potential of two different catalysts was statistically different. A gas diffusion half cell was designed similar to the optical screening cell to obtain current-potential curves of bulk catalysts. The screening results correlated with half cell and fuel cell data, internally validating the method. The combinatorial method was then applied to search for catalysts in the PtRuMoIrRh composition space. The catalysts on the array were prepared by hydrogen reduction of the metals salts on carbon. The most active catalysts were from the Pt enriched regions of the PtRuMoRh quaternary. Bulk catalysts were prepared from the active regions and tested in the gas diffusion half cell. The most active catalysts in the optical screening were also the most active catalysts in the half cell. When any homemade catalysts were compared to commercial PtRu, however, the performance was worse. A high surface area, high catalyst activity synthetic method is the most important factor to reliably screen catalysts for "real world" fuel cell application. High surface area catalysts were tested for direct methanol oxidation activity. The optical screening method was compared with disk electrode, high throughput fuel cell testing, and fuel cell testing. Six catalysts examined included two commercial PtRu catalysts, a Pt catalyst, and three homemade PtRu catalysts of varying activity

STUDY OF SOLVENT AND CATALYST INTERACTIONS IN DIRECT COAL LIQUEFACTION; FINAL

International Nuclear Information System (INIS)

Michael T. Klein; William H. Calkins; Jasna Tomic

2000-01-01

To provide a better understanding of the roles of a solid catalyst and the solvent in Direct Coal Liquefaction, a small reactor was equipped with a porous-walled basket which was permeable to the solvent but was not permeable to the coal or solid catalyst. With this equipment and a high volatile bituminous coal it was found that direct contact between the catalyst in the basket and the coal outside the basket is not required for catalyzed coal liquefaction. The character of the solvent in this system makes a significant difference in the conversion of the coal, the better solvents being strong donor solvents. Because of the extensive use of thermogravimetric analysis in this laboratory, it was noted that the peak temperature for volatiles evolution from coal was a reliable measure of coal rank. Because of this observation, a variety of coals of a range of ranks was investigated. It was shown in this work that measuring the peak temperature for volatiles evolution was a quite precise indicator of rank and correlated closely with the rank value obtained by measuring vitrinite reflectance, a more difficult measurement to make. This prompted the desire to know the composition of the volatile material evolved as a function of coal rank. This was then measured by coupling a TGA to a mass spectrometer using laser activation and photoionization detection TG-PI-MS. The predominant species in volatiles of low rank coal turned out to be phenols with some alkenes. As the rank increases, the relative amounts of alkene and aromatic hydrocarbons increases and the oxygenated species decrease. It was shown that these volatiles were actually pyrolytic products and not volatilization products of the coal. Solvent extraction experiments coupled with Thermogravimetric-photoionization-mass spectrometry (TG-PI-MS) indicated that the low boiling and more extractable material are essentially similar in chemical types to the non-extractable portions but apparently higher molecular weight

Direct Olefination of Alcohols with Sulfones by Using Heterogeneous Platinum Catalysts.

Science.gov (United States)

Siddiki, S M A Hakim; Touchy, Abeda Sultana; Kon, Kenichi; Shimizu, Ken-Ichi

2016-04-18

Carbon-supported Pt nanoparticles (Pt/C) were found to be effective heterogeneous catalysts for the direct Julia olefination of alcohols in the presence of sulfones and KOtBu under oxidant-free conditions. Primary alcohols, including aryl, aliphatic, allyl, and heterocyclic alcohols, underwent olefination with dimethyl sulfone and aryl alkyl sulfones to give terminal and internal olefins, respectively. Secondary alcohols underwent methylenation with dimethyl sulfone. Under 2.5 bar H2, the same reaction system was effective for the transformation of alcohol OH groups to alkyl groups. Structural and mechanistic studies of the terminal olefination system suggested that Pt(0) sites on the Pt metal particles are responsible for the rate-limiting dehydrogenation of alcohols and that KOtBu may deprotonate the sulfone reagent. The Pt/C catalyst was reusable after the olefination, and this method showed a higher turnover number (TON) and a wider substrate scope than previously reported methods, which demonstrates the high catalytic efficiency of the present method. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

A micro alkaline direct ethanol fuel cell with platinum-free catalysts

Science.gov (United States)

Verjulio, R. W.; Alcaide, F.; Álvarez, G.; Sabaté, N.; Torres-Herrero, N.; Esquivel, J. P.; Santander, J.

2013-11-01

This paper presents the fabrication and characterization of a micro alkaline direct ethanol fuel cell. The device has been conceived as a feasibility demonstrator, using microtechnologies for the fabrication of the current collectors and traditional techniques for the membrane electrode assembly production. The fuel cell works in passive mode, as expected for the simplicity required for micro power systems. Non-noble catalysts have been used in order to implement the main advantage of alkaline systems, showing the feasibility of such a device as a potential very-low-cost power device at mini- and micro scales.

Combined UHV/high-pressure catalysis setup for depth-resolved near-surface spectroscopic characterization and catalytic testing of model catalysts

International Nuclear Information System (INIS)

Mayr, Lukas; Klötzer, Bernhard; Penner, Simon; Rameshan, Raffael; Rameshan, Christoph

2014-01-01

An ultra-high vacuum (UHV) setup for “real” and “inverse” model catalyst preparation, depth-resolved near-surface spectroscopic characterization, and quantification of catalytic activity and selectivity under technologically relevant conditions is described. Due to the all-quartz reactor attached directly to the UHV-chamber, transfer of the catalyst for in situ testing without intermediate contact to the ambient is possible. The design of the UHV-compatible re-circulating batch reactor setup allows the study of reaction kinetics under close to technically relevant catalytic conditions up to 1273 K without contact to metallic surfaces except those of the catalyst itself. With the attached differentially pumped exchangeable evaporators and the quartz-microbalance thickness monitoring equipment, a reproducible, versatile, and standardised sample preparation is possible. For three-dimensional near-surface sample characterization, the system is equipped with a hemispherical analyser for X-ray photoelectron spectroscopy (XPS), electron-beam or X-ray-excited Auger-electron spectroscopy, and low-energy ion scattering measurements. Due the dedicated geometry of the X-ray gun (54.7°, “magic angle”) and the rotatable sample holder, depth analysis by angle-resolved XPS measurements can be performed. Thus, by the combination of characterisation methods with different information depths, a detailed three-dimensional picture of the electronic and geometric structure of the model catalyst can be obtained. To demonstrate the capability of the described system, comparative results for depth-resolved sample characterization and catalytic testing in methanol steam reforming on PdGa and PdZn near-surface intermetallic phases are shown

Combined UHV/high-pressure catalysis setup for depth-resolved near-surface spectroscopic characterization and catalytic testing of model catalysts

Science.gov (United States)

Mayr, Lukas; Rameshan, Raffael; Klötzer, Bernhard; Penner, Simon; Rameshan, Christoph

2014-05-01

An ultra-high vacuum (UHV) setup for "real" and "inverse" model catalyst preparation, depth-resolved near-surface spectroscopic characterization, and quantification of catalytic activity and selectivity under technologically relevant conditions is described. Due to the all-quartz reactor attached directly to the UHV-chamber, transfer of the catalyst for in situ testing without intermediate contact to the ambient is possible. The design of the UHV-compatible re-circulating batch reactor setup allows the study of reaction kinetics under close to technically relevant catalytic conditions up to 1273 K without contact to metallic surfaces except those of the catalyst itself. With the attached differentially pumped exchangeable evaporators and the quartz-microbalance thickness monitoring equipment, a reproducible, versatile, and standardised sample preparation is possible. For three-dimensional near-surface sample characterization, the system is equipped with a hemispherical analyser for X-ray photoelectron spectroscopy (XPS), electron-beam or X-ray-excited Auger-electron spectroscopy, and low-energy ion scattering measurements. Due the dedicated geometry of the X-ray gun (54.7°, "magic angle") and the rotatable sample holder, depth analysis by angle-resolved XPS measurements can be performed. Thus, by the combination of characterisation methods with different information depths, a detailed three-dimensional picture of the electronic and geometric structure of the model catalyst can be obtained. To demonstrate the capability of the described system, comparative results for depth-resolved sample characterization and catalytic testing in methanol steam reforming on PdGa and PdZn near-surface intermetallic phases are shown.

Sulfonated reduced graphene oxide as a highly efficient catalyst for direct amidation of carboxylic acids with amines using ultrasonic irradiation.

Science.gov (United States)

Mirza-Aghayan, Maryam; Tavana, Mahdieh Molaee; Boukherroub, Rabah

2016-03-01

Sulfonated reduced graphene oxide nanosheets (rGO-SO3H) were prepared by grafting sulfonic acid-containing aryl radicals onto chemically reduced graphene oxide (rGO) under sonochemical conditions. rGO-SO3H catalyst was characterized by Fourier-transform infrared (FT-IR) spectroscopy, Raman spectroscopy, scanning electron microscopy (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC) and X-ray photoelectron spectroscopy (XPS). rGO-SO3H catalyst was successfully applied as a reusable solid acid catalyst for the direct amidation of carboxylic acids with amines into the corresponding amides under ultrasonic irradiation. The direct sonochemical amidation of carboxylic acid takes place under mild conditions affording in good to high yields (56-95%) the corresponding amides in short reaction times. Copyright © 2015 Elsevier B.V. All rights reserved.

Investigation of a Pt3Sn/C Electro-Catalyst in a Direct Ethanol Fuel Cell Operating at Low Temperatures for Portable Applications

OpenAIRE

Zignani, S. C.; Gonzalez, E. R.; Baglio, V.; Siracusano, S.; Arico, A. S.

2012-01-01

A 20% Pt3Sn/C catalyst was prepared by reduction with formic acid and used in a direct ethanol fuel cell at low temperatures. The electro-catalytic activity of this bimetallic catalyst was compared to that of a commercial 20% Pt/C catalyst. The PtSn catalyst showed better results in the investigated temperature range (30 degrees-70 degrees C). Generally, Sn promotes ethanol oxidation by adsorption of OH species at considerably lower potentials compared to Pt, allowing the occurrence of a bifu...

Development and reactivity tests of Ce-Zr-based Claus catalysts for coal gas cleanup

Energy Technology Data Exchange (ETDEWEB)

No-Kuk Park; Dong Cheul Han; Gi Bo Han; Si Ok Ryu; Tae Jin Lee; Ki Jun Yoon [Yeungnam University, Gyeongbuk (Republic of Korea). National Research Laboratory, School of Chemical Engineering and Technology

2007-09-15

Claus reaction (2H{sub 2}S + SO{sub 2} {leftrightarrow} 3/nS{sub n} + 2H{sub 2}O) was used to clean the gasified coal gas and the reactivity of several metal oxide-based catalysts on Claus reaction was investigated at various operating conditions. In order to convert H{sub 2}S contained in the gasified coal gas to elemental sulfur during Claus reaction, the catalysts having the high activity under the highly reducing condition with the moisture should be developed. CeO{sub 2}, ZrO{sub 2}, and Ce{sub 1-x}Zr{sub x}O{sub 2} catalysts were prepared for Claus reaction and their reactivity changes due to the existence of the reducing gases and H{sub 2}O in the fuel gas was investigated in this study. The Ce-based catalysts shows that their activity was deteriorated by the reduction of the catalyst due to the reducing gases at higher than 220{sup o}C. Meanwhile, the effect of the reducing gases on the catalytic activity was not considerable at low temperature. The activities of all three catalysts were degraded on the condition that the moisture existed in the test gas. Specifically, the Ce-based catalysts were remarkably deactivated by their sulfation. The Ce-Zr-based catalyst had a high catalytic activity when the reducing gases and the moisture co-existed in the simulated fuel gas. The deactivation of the Ce-Zr-based catalyst was not observed in this study. The lattice oxygen of the Ce-based catalyst was used for the oxidation of H{sub 2}S and the lattice oxygen vacancy on the catalyst was contributed to the reduction of SO{sub 2}. ZrO{sub 2} added to the Ce-Zr-based catalyst improved the redox properties of the catalyst in Claus reaction by increasing the mobility of the lattice oxygen of CeO{sub 2}. 21 refs., 14 figs.

Investigation of ethanol electrooxidation on a Pt-Ru-Ni/C catalyst for a direct ethanol fuel cell

Energy Technology Data Exchange (ETDEWEB)

Wang, Zhen-Bo; Yin, Ge-Ping; Zhang, Jian; Sun, Ying-Chao; Shi, Peng-Fei [Department of Applied Chemistry, Harbin Institute of Technology, Harbin (China 150001)

2006-09-29

This research is aimed to improve the utilization and activity of anodic alloy catalysts and thus to lower the contents of noble metals and the catalyst loading on anodes for ethanol electrooxidation. The DEFC anodic catalysts, Pt-Ru-Ni/C and Pt-Ru/C, were prepared by a chemical reduction method. Their performances were tested by using a glassy carbon working electrode and cyclic voltammetric curves, chronoamperometric curves and half cell measurement in a solution of 0.5molL{sup -1} CH{sub 3}CH{sub 2}OH and 0.5molL{sup -1} H{sub 2}SO{sub 4}. The composition of the Pt-Ru-Ni and Pt-Ru surface particles were determined by EDAX analysis. The particle size and lattice parameter of the catalysts were determined by means of X-ray diffraction (XRD). XRD analysis showed that both of the catalysts exhibited face centered cubic structures and had smaller lattice parameters than a Pt-alone catalyst. Their particle sizes were small, about 4.5nm. No significant differences in the ethanol electrooxidation on both electrodes were found using cyclic voltammetry, especially regarding the onset potential for ethanol electrooxidation. The electrochemically active specific areas of the Pt-Ru-Ni/C and Pt-Ru/C catalysts were almost the same. But, the catalytic activity of the Pt-Ru-Ni/C catalyst was higher for ethanol electrooxidation than that of the Pt-Ru/C catalyst. Their tolerance to CO formed as one of the intermediates of ethanol electrooxidation, was better than that of the Pt-Ru/C catalyst. (author)

Direct conversion of cellulose to glycolic acid with a phosphomolybdic acid catalyst in a water medium

KAUST Repository

Zhang, Jizhe

2012-08-03

Direct conversion of cellulose to fine chemicals has rarely been achieved. We describe here an eco-benign route for directly converting various cellulose-based biomasses to glycolic acid in a water medium and oxygen atmosphere in which heteromolybdic acids act as multifunctional catalysts to catalyze the hydrolysis of cellulose, the fragmentation of monosaccharides, and the selective oxidation of fragmentation products. With commercial α-cellulose powder as the substrate, the yield of glycolic acid reaches 49.3%. This catalytic system is also effective with raw cellulosic biomass, such as bagasse or hay, as the starting materials, giving rise to remarkable glycolic acid yields of ∼30%. Our heteropoly acid-based catalyst can be recovered in solid form after reaction by distilling out the products and solvent for reuse, and it exhibits consistently high performance in multiple reaction runs. © 2012 American Chemical Society.

An Investigation of Palladium Oxygen Reduction Catalysts for the Direct Methanol Fuel Cell

Directory of Open Access Journals (Sweden)

G. F. Álvarez

2011-01-01

Full Text Available A comparative study of Pd and Pt was carried out in DMFC using different methanol concentrations and under different operating conditions. Cell performance was compared at methanol concentrations of 1, 3, 5, and 7 M and at temperatures of 20, 40, and 60°C. Homemade Pd nanoparticles were prepared on Vulcan XC-72R using ethylene glycol as the reducing agent at pH 11. The resulting catalyst, Pd/C, with metal nanoparticles of approximately 6 nm diameter, was tested as a cathode catalyst in DMFC. At methanol concentrations of 5 M and higher, the Pd cathode-based cell performed better than that with Pt at 60°C with air.

Pt and Ru X-ray absorption spectroscopy of PtRu anode catalysts in operating direct methanol fuel cells.

Science.gov (United States)

Stoupin, Stanislav; Chung, Eun-Hyuk; Chattopadhyay, Soma; Segre, Carlo U; Smotkin, Eugene S

2006-05-25

In situ X-ray absorption spectroscopy, ex situ X-ray fluorescence, and X-ray powder diffraction enabled detailed core analysis of phase segregated nanostructured PtRu anode catalysts in an operating direct methanol fuel cell (DMFC). No change in the core structures of the phase segregated catalyst was observed as the potential traversed the current onset potential of the DMFC. The methodology was exemplified using a Johnson Matthey unsupported PtRu (1:1) anode catalyst incorporated into a DMFC membrane electrode assembly. During DMFC operation the catalyst is essentially metallic with half of the Ru incorporated into a face-centered cubic (FCC) Pt alloy lattice and the remaining half in an amorphous phase. The extended X-ray absorption fine structure (EXAFS) analysis suggests that the FCC lattice is not fully disordered. The EXAFS indicates that the Ru-O bond lengths were significantly shorter than those reported for Ru-O of ruthenium oxides, suggesting that the phases in which the Ru resides in the catalysts are not similar to oxides.

Durability test with fuel starvation using a Pt/CNF catalyst in PEMFC.

Science.gov (United States)

Jung, Juhae; Park, Byungil; Kim, Junbom

2012-01-05

In this study, a catalyst was synthesized on carbon nanofibers [CNFs] with a herringbone-type morphology. The Pt/CNF catalyst exhibited low hydrophilicity, low surface area, high dispersion, and high graphitic behavior on physical analysis. Electrodes (5 cm2) were prepared by a spray method, and the durability of the Pt/CNF was evaluated by fuel starvation. The performance was compared with a commercial catalyst before and after accelerated tests. The fuel starvation caused carbon corrosion with a reverse voltage drop. The polarization curve, EIS, and cyclic voltammetry were analyzed in order to characterize the electrochemical properties of the Pt/CNF. The performance of a membrane electrode assembly fabricated from the Pt/CNF was maintained, and the electrochemical surface area and cell resistance showed the same trend. Therefore, CNFs are expected to be a good support in polymer electrolyte membrane fuel cells.

Bimetallic Nickel/Ruthenium Catalysts Synthesized by Atomic Layer Deposition for Low-Temperature Direct Methanol Solid Oxide Fuel Cells.

Science.gov (United States)

Jeong, Heonjae; Kim, Jun Woo; Park, Joonsuk; An, Jihwan; Lee, Tonghun; Prinz, Fritz B; Shim, Joon Hyung

2016-11-09

Nickel and ruthenium bimetallic catalysts were heterogeneously synthesized via atomic layer deposition (ALD) for use as the anode of direct methanol solid oxide fuel cells (DMSOFCs) operating in a low-temperature range. The presence of highly dispersed ALD Ru islands over a porous Ni mesh was confirmed, and the Ni/ALD Ru anode microstructure was observed. Fuel cell tests were conducted using Ni-only and Ni/ALD Ru anodes with approximately 350 μm thick gadolinium-doped ceria electrolytes and platinum cathodes. The performance of fuel cells was assessed using pure methanol at operating temperatures of 300-400 °C. Micromorphological changes of the anode after cell operation were investigated, and the content of adsorbed carbon on the anode side of the operated samples was measured. The difference in the maximum power density between samples utilizing Ni/ALD Ru and Pt/ALD Ru, the latter being the best catalyst for direct methanol fuel cells, was observed to be less than 7% at 300 °C and 30% at 350 °C. The improved electrochemical activity of the Ni/ALD Ru anode compared to that of the Ni-only anode, along with the reduction of the number of catalytically active sites due to agglomeration of Ni and carbon formation on the Ni surface as compared to Pt, explains this decent performance.

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.

Spillover effect induced Pt-TiO2/C as ethanol tolerant oxygen reduction reaction catalyst for direct ethanol fuel cells

International Nuclear Information System (INIS)

Meenakshi, S.; Nishanth, K.G.; Sridhar, P.; Pitchumani, S.

2014-01-01

Hypo-hyper-d-electronic interactive nature is used to develop a new carbon supported HT-Pt-TiO 2 composite catalyst comprising Pt and Ti in varying atomic ratio, namely 1:1, 2:1 and 3:1. The electro-catalysts are characterized by XRD, TEM, SEM-EDAX, Cyclic Voltammetry (CV) and Linear sweep voltammetry (LSV) techniques. HT-Pt-TiO 2 /C catalysts exhibit significant improvement in oxygen reduction reaction (ORR) over Pt/C. The effect of composition towards ORR with and without ethanol has been studied. The direct ethanol fuel cell (DEFC) with HT-Pt-TiO 2 /C cathode catalyst exhibits an enhanced peak power density of 41 mW cm −2 , whereas 21 mW cm −2 is obtained for the DEFCs with carbon-supported Pt catalyst operating under identical conditions

Design of a surface alloy catalyst for steam reforming

DEFF Research Database (Denmark)

Besenbacher, F.; Chorkendorff, Ib; Clausen, B.S.

1998-01-01

Detailed studies of elementary chemical processes on well-characterized single crystal surfaces have contributed substantially to the understanding of heterogeneous catalysis. insight into the structure of surface alloys combined with an understanding of the relation between the surface compositi...... and reactivity is shown to lead directly to new ideas for catalyst design, The feasibility of such an approach is illustrated by the synthesis, characterization, and tests of a high-surface area gold-nickel catalyst for steam reforming....

Confidence Testing of Shell 405 and S-405 Catalysts in a Monopropellant Hydrazine Thruster

Science.gov (United States)

McRight, Patrick; Popp, Chris; Pierce, Charles; Turpin, Alicia; Urbanchock, Walter; Wilson, Mike

2005-01-01

As part of the transfer of catalyst manufacturing technology from Shell Chemical Company (Shell 405 catalyst manufactured in Houston, Texas) to Aerojet (S-405 manufactured in Redmond, Washington), Aerojet demonstrated the equivalence of S-405 and Shell 405 at beginning of life. Some US aerospace users expressed a desire to conduct a preliminary confidence test to assess end-of-life characteristics for S-405. NASA Marshall Space Flight Center (MSFC) and Aerojet entered a contractual agreement in 2004 to conduct a confidence test using a pair of 0.2-lbf MR-103G monopropellant hydrazine thrusters, comparing S-405 and Shell 405 side by side. This paper summarizes the formulation of this test program, explains the test matrix, describes the progress of the test, and analyzes the test results. This paper also includes a discussion of the limitations of this test and the ramifications of the test results for assessing the need for future qualification testing in particular hydrazine thruster applications.

Synthesis and characterization of Pt-Sn-Ni alloys to application as catalysts for direct ethanol fuel cells

International Nuclear Information System (INIS)

Silva, E.L. da; Correa, P.S.; Oliveira, E.L. de; Takimi, A.S.; Malfatti, C.F.; Radtke, C.

2010-01-01

Direct ethanol fuel cells (DEFCs) have been the focus of recent research due its application in mobile energy sources. In order to obtain the maximum efficiency from these systems, it is necessary the total ethanol oxidation, which implies in C-C bond break. Different catalysts described in literature are employed with this intent. This work consists in studying PtSnNi catalysts supported on carbon Vulcan XC72R, to application in DEFCs. Thus, it was used the impregnation/reduction method, varying the atomic proportion among Pt, Sn and Ni. The alloys were characterized by X-Ray Diffraction, Cyclic Voltammetry and Transmission Microscopy. Preliminary results show that predominant structure on the catalysts is the face centered cubic platinum and the densities currents are dependent on the platinum amount. (author)

Alkali resistant Ni-loaded yolk-shell catalysts for direct internal reforming in molten carbonate fuel cells

Science.gov (United States)

Jang, Won-Jun; Hong, Young Jun; Kim, Hak-Min; Shim, Jae-Oh; Roh, Hyun-Seog; Kang, Yun Chan

2017-06-01

A facile and scalable spray pyrolysis process is applied to synthesize multi-shelled Ni-loaded yolk-shell catalysts on various supports (Al2O3, CeO2, ZrO2, and La(OH)3). The prepared catalysts are applied to direct internal reforming (DIR) in a molten carbonate fuel cell (MCFC). Even on exposure to alkali hydroxide vapors, the Ni-loaded yolk-shell catalysts remain highly active for DIR-MCFCs. The Ni@Al2O3 microspheres show the highest conversion (92%) of CH4 and the best stability among the prepared Ni-loaded yolk-shell catalysts. Although the initial CH4 conversion of the Ni@ZrO2 microspheres is higher than that of the Ni@CeO2 microspheres, the Ni@CeO2 microspheres are more stable. The catalytic performance is strongly dependent on the surface area and acidity and also partly dependent on the reducibility. The acidic nature of Al2O3 combined with its high surface area and yolk-shell structure enhances the adsorption of CH4 and resistance against alkali poisoning, resulting in efficient DIR-MCFC reactions.

Direct observation of surface reconstruction and termination on a complex metal oxide catalyst by electron microscopy

KAUST Repository

Zhu, Yihan

2012-03-19

On the surface: The surface reconstruction of an MoVTeO complex metal oxide catalyst was observed directly by various electron microscopic techniques and the results explain the puzzling catalytic behavior. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

PILOT TESTING OF MERCURY OXIDATION CATALYSTS FOR UPSTREAM OF WET FGD SYSTEMS

International Nuclear Information System (INIS)

Gary M. Blythe

2002-01-01

The objective of this project is to demonstrate at pilot scale the use of solid honeycomb catalysts to promote the oxidation of elemental mercury in the flue gas from coal combustion. The project is being funded by the U.S. DOE National Energy Technology Laboratory under Cooperative Agreement DE-FC26-01NT41185. EPRI, Great River Energy (GRE), and City Public Service (CPS) of San Antonio are project co-funders. URS Group is the prime contractor. The mercury catalytic oxidation process under development uses catalyst materials applied to honeycomb substrates to promote the oxidation of elemental mercury in the flue gas from coal-fired power plants that have wet lime or limestone flue gas desulfurization (FGD) systems. Oxidized mercury is removed in the wet FGD absorbers and co-precipitates in a stable form with the byproducts from the FGD system. The co-precipitated mercury does not appear to adversely affect the disposal or reuse properties of the FGD byproduct. The current project will test previously identified, effective catalyst materials at a larger, pilot scale and in a commercial form, so as to provide engineering data for future full-scale designs. The pilot-scale tests will continue for up to 14 months at each of two sites to provide longer-term catalyst life data. This is the first full reporting period for the subject Cooperative Agreement. During this period, most of the project efforts were related to project initiation and planning. There is no significant technical progress to report for the current period

PREPARATION, CHARACTERIZATION AND CATALYTIC ACTIVITY TEST OF CoMo/ZnO CATALYST ON ETHANOL CONVERSION USING STEAM REFORMING METHOD

Directory of Open Access Journals (Sweden)

Wega Trisunaryanti

2010-06-01

Full Text Available Preparation, characterization and catalytic activity test of CoMo/ZnO catalyst for steam reforming of ethanol have been investigated. The catalysts preparation was carried out by impregnation of Co and/or Mo onto ZnO sample. Water excess was used in ethanol feed for steam reforming process under mol ratio of ethanol:water (1:10. Characterizations of catalysts were conducted by analysis of metal content using Atomic Absorption Spectroscopy (AAS. Determination of catalysts acidity was conducted by gravimetric method of adsorption of pyridine base. Catalytic activity test on ethanol conversion using steam reforming method was conducted in a semi-flow reactor system, at a temperature of 400 oC, for 1.5 h under N2 flow rate of 10 mL/min. Gas product was analyzed by gas chromatograph with TCD system. The results of catalysts characterizations showed that the impregnation of Co and/or Mo metals on ZnO sample increased its acidity and specific surface area. The content of Co in Co/ZnO and CoMo/ZnO catalysts was 1.14 and 0.49 wt%. The Mo content in CoMo/ZnO catalyst was 0.36 wt%. The catalytic activity test result on ethanol conversion showed that the ZnO, Co/ZnO, and CoMo/ZnO catalysts produced gas fraction of 16.73, 28.53, and 35.53 wt%, respectively. The coke production of ZnO, Co/ZnO, and CoMo/ZnO catalysts was 0.86, 0.24, and 0.08 wt%, respectively. The gas products consisted mainly of hydrogen.   Keywords: CoMo/ZnO catalyst, steam reforming, ethanol

The Carbonation of Wollastonite: A Model Reaction to Test Natural and Biomimetic Catalysts for Enhanced CO2 Sequestration

Directory of Open Access Journals (Sweden)

Fulvio Di Lorenzo

2018-05-01

Full Text Available One of the most promising strategies for the safe and permanent disposal of anthropogenic CO2 is its conversion into carbonate minerals via the carbonation of calcium and magnesium silicates. However, the mechanism of such a reaction is not well constrained, and its slow kinetics is a handicap for the implementation of silicate mineral carbonation as an effective method for CO2 capture and storage (CCS. Here, we studied the different steps of wollastonite (CaSiO3 carbonation (silicate dissolution → carbonate precipitation as a model CCS system for the screening of natural and biomimetic catalysts for this reaction. Tested catalysts included carbonic anhydrase (CA, a natural enzyme that catalyzes the reversible hydration of CO2(aq, and biomimetic metal-organic frameworks (MOFs. Our results show that dissolution is the rate-limiting step for wollastonite carbonation. The overall reaction progresses anisotropically along different [hkl] directions via a pseudomorphic interface-coupled dissolution–precipitation mechanism, leading to partial passivation via secondary surface precipitation of amorphous silica and calcite, which in both cases is anisotropic (i.e., (hkl-specific. CA accelerates the final carbonate precipitation step but hinders the overall carbonation of wollastonite. Remarkably, one of the tested Zr-based MOFs accelerates the dissolution of the silicate. The use of MOFs for enhanced silicate dissolution alone or in combination with other natural or biomimetic catalysts for accelerated carbonation could represent a potentially effective strategy for enhanced mineral CCS.

A micro alkaline direct ethanol fuel cell with platinum-free catalysts

International Nuclear Information System (INIS)

Verjulio, R W; Sabaté, N; Torres-Herrero, N; Esquivel, J P; Santander, J; Alcaide, F; Álvarez, G

2013-01-01

This paper presents the fabrication and characterization of a micro alkaline direct ethanol fuel cell. The device has been conceived as a feasibility demonstrator, using microtechnologies for the fabrication of the current collectors and traditional techniques for the membrane electrode assembly production. The fuel cell works in passive mode, as expected for the simplicity required for micro power systems. Non-noble catalysts have been used in order to implement the main advantage of alkaline systems, showing the feasibility of such a device as a potential very-low-cost power device at mini- and micro scales. (paper)

Carbonaceous deposits on naptha reforming catalysts

International Nuclear Information System (INIS)

Redwan, D.S.

1999-01-01

Carbonaceous deposits on naphtha reforming catalysts play a decisive role in limiting process performance. The deposits negatively after catalyst activity, selectivity and the production cycle of a semi regenerative reformer. The magnitude of negative effect of those deposits is directly proportional to their amounts and complexity. Investigations on used reforming catalysts samples reveal that the amount and type (complexity of the chemical nature) of carbonaceous deposits are directly proportional to the catalysts life on stream and the severity of operating conditions. In addition, the combustibility behavior of carbonaceous deposits on the catalyst samples taken from different reformers are found to be different. Optimal carbon removal, for in situ catalyst regeneration, requires the specific conditions be developed, based on the results of well designed and properly performed investigations of the amount and type of carbonaceous deposits. (author)

Platinum and palladium nano-structured catalysts for polymer electrolyte fuel cells and direct methanol fuel cells.

Science.gov (United States)

Long, Nguyen Viet; Thi, Cao Minh; Yong, Yang; Nogami, Masayuki; Ohtaki, Michitaka

2013-07-01

In this review, we present the synthesis and characterization of Pt, Pd, Pt based bimetallic and multi-metallic nanoparticles with mixture, alloy and core-shell structure for nano-catalysis, energy conversion, and fuel cells. Here, Pt and Pd nanoparticles with modified nanostructures can be controllably synthesized via chemistry and physics for their uses as electro-catalysts. The cheap base metal catalysts can be studied in the relationship of crystal structure, size, morphology, shape, and composition for new catalysts with low cost. Thus, Pt based alloy and core-shell catalysts can be prepared with the thin Pt and Pt-Pd shell, which are proposed in low and high temperature proton exchange membrane fuel cells (PEMFCs), and direct methanol fuel cells (DMFCs). We also present the survey of the preparation of Pt and Pd based catalysts for the better catalytic activity, high durability, and stability. The structural transformations, quantum-size effects, and characterization of Pt and Pd based catalysts in the size ranges of 30 nm (1-30 nm) are presented in electro-catalysis. In the size range of 10 nm (1-10 nm), the pure Pt catalyst shows very large surface area for electro-catalysis. To achieve homogeneous size distribution, the shaped synthesis of the polyhedral Pt nanoparticles is presented. The new concept of shaping specific shapes and morphologies in the entire nano-scale from nano to micro, such as polyhedral, cube, octahedra, tetrahedra, bar, rod, and others of the nanoparticles is proposed, especially for noble and cheap metals. The uniform Pt based nanosystems of surface structure, internal structure, shape, and morphology in the nanosized ranges are very crucial to next fuel cells. Finally, the modifications of Pt and Pd based catalysts of alloy, core-shell, and mixture structures lead to find high catalytic activity, durability, and stability for nano-catalysis, energy conversion, fuel cells, especially the next large-scale commercialization of next

Congressionally Directed Project for Passive NOx Removal Catalysts Research

Energy Technology Data Exchange (ETDEWEB)

Schneider, William [Univ. of Notre Dame, IN (United States)

2014-12-29

The Recipient proposes to produce new scientific and technical knowledge and tools to enable the discovery and deployment of highly effective materials for the selective catalytic reduction (SCR) of nitrogen oxides (NOx) from lean combustion exhaust. A second goal is to demonstrate a closely coupled experimental and computational approach to heterogeneous catalysis research. These goals will be met through the completion of four primary technical objectives: First, an in-depth kinetic analysis will be performed on two prominent classes of NOx SCR catalysts, Fe- and Cu-exchanged beta and ZSM-5 zeolites, over a wide range of catalyst formulation and under identical, high conversion conditions as a function of gas phase composition. Second, the nanoscale structure and adsorption chemistry of these high temperature (HT) and low temperature (LT) catalysts will be determined using in situ and operando spectroscopy under the same reaction conditions. Third, first-principles molecular simulations will be used to model the metal-zeolite active sites, their adsorption chemistry, and key steps in catalytic function. Fourth, this information will be integrated into chemically detailed mechanistic and kinetic descriptions and models of the operation of these well- defined NOx SCR catalysts under practically relevant reaction conditions. The new knowledge and models that derive from this work will be published in the scientific literature.

Preparation, characterization and testing of SiC-based catalytic sponges as structured catalysts for Fischer-Tropsch synthesis

Energy Technology Data Exchange (ETDEWEB)

Baudry, A.; Schaub, G. [Karlsruhe Institute of Technology (KIT), Karlsruhe (Germany). Engler-Bunte-Inst.

2011-07-01

Solid sponges (open-cell foams) may be used as catalyst support, due to favorable thermal properties and low pressure drop. As an example, they may lead to improved temperature control in Fischer-Tropsch applications, if compared to fixed beds of catalyst particles. The aim of this study was to develop and test a wet method for impregnating ceramic foam materials with a CoRe/{gamma}-Al{sub 2}O{sub 3} catalyst. Defined catalyst layers were generated on 20 ppi SiC-sponges. Resulting catalytic activities are nearly identical to those of the corresponding powder catalyst material. The difference observed can be explained by either mass transfer limitation or backmixing in the fixed bed configuration used. (orig.)

Ruthenium–Platinum Catalysts and Direct Methanol Fuel Cells (DMFC: A Review of Theoretical and Experimental Breakthroughs

Directory of Open Access Journals (Sweden)

Ana S. Moura

2017-02-01

Full Text Available The increasing miniaturization of devices creates the need for adequate power sources and direct methanol fuel cells (DMFC are a strong option in the various possibilities under current development. DMFC catalysts are mostly based on platinum, for its outperformance in three key areas (activity, selectivity and stability within methanol oxidation framework. However, platinum poisoning with products of methanol oxidation led to the use of alloys. Ruthenium–platinum alloys are preferred catalysts active phases for methanol oxidation from an industrial point of view and, indeed, ruthenium itself is a viable catalyst for this reaction. In addition, the route of methanol decomposition is crucial in the goal of producing H2 from water reaction with methanol. However, the reaction pathway remains elusive and new approaches, namely in computational methods, have been ensued to determine it. This article reviews the various recent theoretical approaches for determining the pathway of methanol decomposition, and systematizes their validation with experimental data, within methodological context.

Radio-Frequency-Based NH₃-Selective Catalytic Reduction Catalyst Control: Studies on Temperature Dependency and Humidity Influences.

Science.gov (United States)

Dietrich, Markus; Hagen, Gunter; Reitmeier, Willibald; Burger, Katharina; Hien, Markus; Grass, Philippe; Kubinski, David; Visser, Jaco; Moos, Ralf

2017-07-12

The upcoming more stringent automotive emission legislations and current developments have promoted new technologies for more precise and reliable catalyst control. For this purpose, radio-frequency-based (RF) catalyst state determination offers the only approach for directly measuring the NH₃ loading on selective catalytic reduction (SCR) catalysts and the state of other catalysts and filter systems. Recently, the ability of this technique to directly control the urea dosing on a current NH₃ storing zeolite catalyst has been demonstrated on an engine dynamometer for the first time and this paper continues that work. Therefore, a well-known serial-type and zeolite-based SCR catalyst (Cu-SSZ-13) was investigated under deliberately chosen high space velocities. At first, the full functionality of the RF system with Cu-SSZ-13 as sample was tested successfully. By direct RF-based NH₃ storage control, the influence of the storage degree on the catalyst performance, i.e., on NO x conversion and NH₃ slip, was investigated in a temperature range between 250 and 400 °C. For each operation point, an ideal and a critical NH₃ storage degree was found and analyzed in the whole temperature range. Based on the data of all experimental runs, temperature dependent calibration functions were developed as a basis for upcoming tests under transient conditions. Additionally, the influence of exhaust humidity was observed with special focus on cold start water and its effects to the RF signals.

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.

Cu-ZSM-5, Cu-ZSM-11, and Cu-ZSM-12 Catalysts for Direct NO Decomposition

DEFF Research Database (Denmark)

Kustova, Marina; Kustov, Arkadii; Christiansen, Sofie E.

2006-01-01

Cu-ZSM-5 has for many years been recognized as a unique catalyst for direct NO decomposition. Here, it is discovered that both Cu-ZSM-11 and Cu-ZSM-12 are about twice as active as Cu-ZSM-5. This difference is attributed to the active sites located almost exclusively in the straight zeolite pores...

Radio-Frequency-Controlled Urea Dosing for NH₃-SCR Catalysts: NH₃ Storage Influence to Catalyst Performance under Transient Conditions.

Science.gov (United States)

Dietrich, Markus; Hagen, Gunter; Reitmeier, Willibald; Burger, Katharina; Hien, Markus; Grass, Philippe; Kubinski, David; Visser, Jaco; Moos, Ralf

2017-11-28

Current developments in exhaust gas aftertreatment led to a huge mistrust in diesel driven passenger cars due to their NO x emissions being too high. The selective catalytic reduction (SCR) with ammonia (NH₃) as reducing agent is the only approach today with the capability to meet upcoming emission limits. Therefore, the radio-frequency-based (RF) catalyst state determination to monitor the NH₃ loading on SCR catalysts has a huge potential in emission reduction. Recent work on this topic proved the basic capability of this technique under realistic conditions on an engine test bench. In these studies, an RF system calibration for the serial type SCR catalyst Cu-SSZ-13 was developed and different approaches for a temperature dependent NH₃ storage were determined. This paper continues this work and uses a fully calibrated RF-SCR system under transient conditions to compare different directly measured and controlled NH₃ storage levels, and NH₃ target curves. It could be clearly demonstrated that the right NH₃ target curve, together with a direct control on the desired level by the RF system, is able to operate the SCR system with the maximum possible NO x conversion efficiency and without NH₃ slip.

Reusability and Stability Tests of Calcium Oxide Based Catalyst (K2O/CaO-ZnO for Transesterification of Soybean Oil to Biodiesel

Directory of Open Access Journals (Sweden)

Istadi Istadi

2016-03-01

Full Text Available This paper was purposed for testing reusability and stability of calcium oxide-based catalyst (K2O/CaO-ZnO over transesterification reaction of soybean oil with methanol to produce biodiesel. The K2O/CaO-ZnO catalyst was synthesized by co-precipitation method of calcium and zinc nitrates followed by impregnation of potassium nitrate. The fresh and used catalysts were tested after regeneration. The catalysts were characterized by Scanning Electron Microscopy (SEM, X-ray Diffraction (XRD, and BET Surface Area in order to compare the catalyst structure between the fresh and used catalysts. The catalyst testing in transesterification proses was carried out at following operating conditions, i.e. catalyst weight of 6 wt.%, oil to methanol mole ratio of 1:15, and temperature of 60 oC. In addition, metal oxide leaching of K2O/CaO-ZnO catalyst during reaction was also tested. From the results, the catalysts exhibited high catalytic activity (80% fatty acid methyl ester (FAME yield after three-cycles of usage and acceptable reusability after regeneration. The catalyst also showed acceptable stability of catalytic activity, even after three-cycles of usage. Copyright © 2016 BCREC GROUP. All rights reserved Received: 10th November 2015; Revised: 16th January 2016; Accepted: 16th January 2016 How to Cite: Istadi, I., Mabruro, U., Kalimantini, B.A.,  Buchori, L., Anggoro, D.D. (2016. Reusability and Stability Tests of Calcium Oxide Based Catalyst (K2O/CaO-ZnO for Transesterification of Soybean Oil to Biodiesel. Bulletin of Chemical Reaction Engineering & Catalysis, 11 (1: 34-39. (doi:10.9767/bcrec.11.1.413.34-39 Permalink/DOI: http://dx.doi.org/10.9767/bcrec.11.1.413.34-39

Use of hydrophobic Pt-catalysts in tritium removal from effluents

International Nuclear Information System (INIS)

Gheorghe, Ionita; Popescu, Irina; Stefanescu, Ioan; Steflea, Dumitru; Varlam, Carmen

2002-01-01

Based on the long experience of the authors, in the preparation, testing and evaluation of the performances of hydrophobic catalysts, and based on the reviewed references, this paper presents up-to-date R and D activities on the application of the hydrophobic catalysts in tritium removal from nuclear effluents. Tritium removal from the heavy water reactor and nuclear reprocessing plant, the cleanup of atmosphere and gaseous effluents by hydrogen-oxygen recombination, removal of oxygen dissolved in water are presented and discussed. Unlike the conventional hydrophilic catalysts, the hydrophobic catalysts keep a high catalytic activity and stability, even under the direct contact to liquid water or in presence of saturated humidity. A large diversity of catalyst types (over 100 catalysts) was prepared and tested in order to make them feasible for such processes. The objectives of the review are: - to provide a database for selection of the most appropriate catalyst and catalytic packing for above mentioned processes; - the designing and operation of reactor packed with hydrophobic catalysts; - to evaluate the potentiality of hydrophobic Pt-catalysts in the present and future applications. The most important results are the following: - the hydrophobic Pt-catalysts packed in the trickle bed or separated bed reactors, showed a high catalytic activity and long stability; - the utilization of the hydrophobic Pt-catalysts for the hydrogen isotopes (tritium and deuterium) separation and for hydrogen-oxygen recombination in nuclear field was entirely confirmed on industrial scale; - the improvement of the inner geometry of the reactors and of the composition of mixed catalytic packing as well as the evaluation of performances of separation processes constitute a major contribution of the authors; - the extension of the utilization of the hydrophobic Pt-catalysts in the oxidation of volatile organic compounds from wastewater; - the removal of dissolved oxygen, and deuterium

Radio-Frequency-Based NH3-Selective Catalytic Reduction Catalyst Control: Studies on Temperature Dependency and Humidity Influences

Directory of Open Access Journals (Sweden)

Markus Dietrich

2017-07-01

Full Text Available The upcoming more stringent automotive emission legislations and current developments have promoted new technologies for more precise and reliable catalyst control. For this purpose, radio-frequency-based (RF catalyst state determination offers the only approach for directly measuring the NH3 loading on selective catalytic reduction (SCR catalysts and the state of other catalysts and filter systems. Recently, the ability of this technique to directly control the urea dosing on a current NH3 storing zeolite catalyst has been demonstrated on an engine dynamometer for the first time and this paper continues that work. Therefore, a well-known serial-type and zeolite-based SCR catalyst (Cu-SSZ-13 was investigated under deliberately chosen high space velocities. At first, the full functionality of the RF system with Cu-SSZ-13 as sample was tested successfully. By direct RF-based NH3 storage control, the influence of the storage degree on the catalyst performance, i.e., on NOx conversion and NH3 slip, was investigated in a temperature range between 250 and 400 °C. For each operation point, an ideal and a critical NH3 storage degree was found and analyzed in the whole temperature range. Based on the data of all experimental runs, temperature dependent calibration functions were developed as a basis for upcoming tests under transient conditions. Additionally, the influence of exhaust humidity was observed with special focus on cold start water and its effects to the RF signals.

Radio-Frequency-Based NH3-Selective Catalytic Reduction Catalyst Control: Studies on Temperature Dependency and Humidity Influences

Science.gov (United States)

Dietrich, Markus; Hagen, Gunter; Reitmeier, Willibald; Burger, Katharina; Hien, Markus; Grass, Philippe; Kubinski, David; Visser, Jaco; Moos, Ralf

2017-01-01

The upcoming more stringent automotive emission legislations and current developments have promoted new technologies for more precise and reliable catalyst control. For this purpose, radio-frequency-based (RF) catalyst state determination offers the only approach for directly measuring the NH3 loading on selective catalytic reduction (SCR) catalysts and the state of other catalysts and filter systems. Recently, the ability of this technique to directly control the urea dosing on a current NH3 storing zeolite catalyst has been demonstrated on an engine dynamometer for the first time and this paper continues that work. Therefore, a well-known serial-type and zeolite-based SCR catalyst (Cu-SSZ-13) was investigated under deliberately chosen high space velocities. At first, the full functionality of the RF system with Cu-SSZ-13 as sample was tested successfully. By direct RF-based NH3 storage control, the influence of the storage degree on the catalyst performance, i.e., on NOx conversion and NH3 slip, was investigated in a temperature range between 250 and 400 °C. For each operation point, an ideal and a critical NH3 storage degree was found and analyzed in the whole temperature range. Based on the data of all experimental runs, temperature dependent calibration functions were developed as a basis for upcoming tests under transient conditions. Additionally, the influence of exhaust humidity was observed with special focus on cold start water and its effects to the RF signals. PMID:28704929

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

Science.gov (United States)

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

2018-09-01

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

Direct upgrading of fast pyrolysis lignin vapor over the HZSM-5 catalyst

DEFF Research Database (Denmark)

Zhou, Guofeng; Jensen, Peter Arendt; Le, Duy M.

2016-01-01

is reduced from 27.6 wt%daf without a catalyst to 5.7 wt%daf (600 °C catalyst temperature). The energy recovery in the liquid organics is 8.7% (600 °C catalyst temperature), compared to the 33.0% energy recovery in the organic liquid from the non-catalytic run. Oxygen is removed from the pyrolysis vapor...

Direct synthesis of Pt-free catalyst on gas diffusion layer of fuel cell and usage of high boiling point fuels for efficient utilization of waste heat

International Nuclear Information System (INIS)

Nandan, Ravi; Goswami, Gopal Krishna; Nanda, Karuna Kar

2017-01-01

Graphical abstract: Direct-grown boron-doped carbon nanotubes on gas-diffusion layer as efficient Pt-free cathode catalyst for alcohol fuel cells, high boiling point fuels used to obtain hot fuels for the enhancement of cell performance that paves the way for the utilization of waste heat. Display Omitted -- Highlights: •One-step direct synthesis of boron-doped carbon nanotubes (BCNTs) on gas diffusion layer (GDL). •Home built fuel-cell testing using BCNTs on GDL as Pt-free cathode catalyst. •BCNTs exhibit concentration dependent oxygen reduction reaction and the cell performance. •Effective utilization of waste heat to raise the fuel temperature. •Fuel selectivity to raise the fuel temperature and the overall performance of the fuel cells. -- Abstract: Gas diffusion layers (GDL) and electrocatalysts are integral parts of fuel cells. It is, however, a challenging task to grow Pt-free robust electrocatalyst directly on GDL for oxygen reduction reaction (ORR) – a key reaction in fuel cells. Here, we demonstrate that boron-doped carbon nanotubes (BCNTs) grown directly on gas-diffusion layer (which avoid the need of ionomer solution used for catalyst loading) can be used as efficient Pt-free catalyst in alcohol fuel cells. Increase in boron concentration improves the electrochemical ORR activity in terms of onset and ORR peak positions, half-wave potentials and diffusion-limited current density that ensure the optimization of the device performance. The preferential 4e − pathway, excellent cell performance, superior tolerance to fuel crossover and long-term stability makes directly grown BCNTs as an efficient Pt-free cathode catalyst for cost-effective fuel cells. The maximum power density of the fuel cell is found to increase monotonically with boron concentration. In addition to the application of BCNTs in fuel cell, we have introduced the concept of hot fuels so that waste heat can effectively be used and external power sources can be avoided. The fuel

High-Activity Dealloyed Catalysts

Energy Technology Data Exchange (ETDEWEB)

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

2014-09-30

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

The Effect of Annealing Temperature on Nickel on Reduced Graphene Oxide Catalysts on Urea Electrooxidation

International Nuclear Information System (INIS)

Glass, Dean E.; Galvan, Vicente; Prakash, G.K. Surya

2017-01-01

Highlights: •Nickel was reduced on graphene oxide and annealed under argon from 300 to 700 °C. •Nickel was oxidized from the removal of oxygen groups on the graphene oxide. •Higher annealed catalysts displayed decreased urea electrooxidation currents. •Micro direct urea/hydrogen peroxide fuel cells were employed for the first time. •Ni/rGO catalysts displayed enhanced fuel cell performance than the bare nickel. -- Abstract: The annealing temperature effects on nickel on reduced graphene oxide (Ni/rGO) catalysts for urea electrooxidation were investigated. Nickel chloride was directly reduced in an aqueous solution of graphene oxide (GO) followed by annealing under argon at 300, 400, 500, 600, and 700 °C, respectively. X-ray Diffraction (XRD) patterns revealed an increase in the crystallite size of the nickel nanoparticles while the Raman spectra displayed an increase in the graphitic disorder of the reduced graphene oxide at higher annealing temperatures due to the removal of oxygen functional groups. The Ni/rGO catalysts annealed at higher temperatures displayed oxidized nickel surface characteristics from the Ni 2p X-ray Photoelectron Spectra (XPS) due to the oxidation of the nickel from the oxygen functional groups in the graphitic lattice. In the half-cell testing, the onset potential of urea electrooxidation decreased while the urea electrooxidation currents decreased as the annealing temperature was increased. The nickel catalyst annealed at 700 °C displayed a 31% decrease in peak power density while the catalyst annealed at 300 °C displayed a 13% increase compared with the unannealed Ni/rGO catalyst in the micro direct urea/hydrogen peroxide fuel cells tests.

Atomic layer deposition of ruthenium surface-coating on porous platinum catalysts for high-performance direct ethanol solid oxide fuel cells

Science.gov (United States)

Jeong, Heon Jae; Kim, Jun Woo; Jang, Dong Young; Shim, Joon Hyung

2015-09-01

Pt-Ru bi-metallic catalysts are synthesized by atomic layer deposition (ALD) of Ru surface-coating on sputtered Pt mesh. The catalysts are evaluated in direct ethanol solid oxide fuel cells (DESOFCs) in the temperature range of 300-500 °C. Island-growth of the ALD Ru coating is confirmed by transmission electron microscopy and X-ray photoelectron spectroscopy (XPS) analyses. The performance of the DESOFCs is evaluated based on the current-voltage output and electrochemical impedance spectroscopy. Genuine reduction of the polarization impedance, and enhanced power output with improved surface kinetics are achieved with the optimized ALD Ru surface-coating compared to bare Pt. The chemical composition of the Pt/ALD Ru electrode surface after fuel cell operation is analyzed via XPS. Enhanced cell performance is clearly achieved, attributed to the effective Pt/ALD Ru bi-metallic catalysis, including oxidation of Cdbnd O by Ru, and de-protonation of ethanol and cleavage of C-C bonds by Pt, as supported by surface morphology analysis which confirms formation of a large amount of carbon on bare Pt after the ethanol-fuel-cell test.

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.

Direct fabrication of metal-free hollow graphene balls with a self-supporting structure as efficient cathode catalysts of fuel cell

Energy Technology Data Exchange (ETDEWEB)

Lu, Yanqi; Liu, Mingda; Nie, Huagui, E-mail: huaguinie@126.com; Gu, Cancan; Liu, Ming; Yang, Zhi, E-mail: yang201079@126.com; Yang, Keqin; Chen, Xi’an; Huang, Shaoming, E-mail: smhuang@wzu.edu.cn [Wenzhou University, Nanomaterials and Chemistry Key Laboratory (China)

2016-06-15

Despite the good progress in developing carbon catalysts for oxygen reduction reaction (ORR), the current metal-free carbon catalysts are still far from satisfactory for large-scale applications of fuel cell. Developing hollow graphene balls with a self-supporting structure is considered to be an ideal method to inhibit graphene stacking and improve their catalytic performance. Herein, we fabricated metal-free hollow graphene balls with a self-supporting structure, through using a new strategy that involves direct metal-free catalytic growth from assembly of SiO{sub 2} spheres. To our knowledge, although much researches involving the synthesis of graphene balls have been reported, investigations into the direct metal-free catalytic growth of hollow graphene balls are rare. Furthermore, the electrocatalytic performance shows that the resulting hollow graphene balls have significantly high catalytic activity. More importantly, such catalysts also possess much improved stability and better methanol tolerance in alkaline media during the ORR compared with commercial Pt/C catalysts. The outstanding performances coupled with an easy and inexpensive preparing method indicated the great potential of the hollow graphene balls with a self-supporting structure in large-scale applications of fuel cell.Graphical AbstractHollow graphene balls with a self-supporting structure have been successfully fabricated, through using a new strategy that involves direct metal-free catalytic growth from 3D assembly of SiO{sub 2} spheres. The hollow graphene balls can exhibit a high catalytic activity, long-term stability, and an excellent methanol tolerance for the oxygen reduction reaction.

Direct fabrication of metal-free hollow graphene balls with a self-supporting structure as efficient cathode catalysts of fuel cell

International Nuclear Information System (INIS)

Lu, Yanqi; Liu, Mingda; Nie, Huagui; Gu, Cancan; Liu, Ming; Yang, Zhi; Yang, Keqin; Chen, Xi’an; Huang, Shaoming

2016-01-01

Despite the good progress in developing carbon catalysts for oxygen reduction reaction (ORR), the current metal-free carbon catalysts are still far from satisfactory for large-scale applications of fuel cell. Developing hollow graphene balls with a self-supporting structure is considered to be an ideal method to inhibit graphene stacking and improve their catalytic performance. Herein, we fabricated metal-free hollow graphene balls with a self-supporting structure, through using a new strategy that involves direct metal-free catalytic growth from assembly of SiO_2 spheres. To our knowledge, although much researches involving the synthesis of graphene balls have been reported, investigations into the direct metal-free catalytic growth of hollow graphene balls are rare. Furthermore, the electrocatalytic performance shows that the resulting hollow graphene balls have significantly high catalytic activity. More importantly, such catalysts also possess much improved stability and better methanol tolerance in alkaline media during the ORR compared with commercial Pt/C catalysts. The outstanding performances coupled with an easy and inexpensive preparing method indicated the great potential of the hollow graphene balls with a self-supporting structure in large-scale applications of fuel cell.Graphical AbstractHollow graphene balls with a self-supporting structure have been successfully fabricated, through using a new strategy that involves direct metal-free catalytic growth from 3D assembly of SiO_2 spheres. The hollow graphene balls can exhibit a high catalytic activity, long-term stability, and an excellent methanol tolerance for the oxygen reduction reaction

Highly Durable Platinum Single-Atom Alloy Catalyst for Electrochemical Reactions

DEFF Research Database (Denmark)

Kim, Jiwhan; Roh, Chi-Woo; Sahoo, Suman Kalyan

2018-01-01

Single atomic Pt catalyst can offer efficient utilization of the expensive platinum and provide unique selectivity because it lacks ensemble sites. However, designing such a catalyst with high Pt loading and good durability is very challenging. Here, single atomic Pt catalyst supported on antimony...... functional theory calculations show that replacing Sb sites with Pt atoms in the bulk phase or at the surface of SbSn or ATO is energetically favorable. The Pt1/ATO shows superior activity and durability for formic acid oxidation reaction, compared to a commercial Pt/C catalyst. The single atomic Pt...... structure is retained even after a harsh durability test, which is performed by repeating cyclic voltammetry in the range of 0.05–1.4 V for 1800 cycles. A full cell is fabricated for direct formic acid fuel cell using the Pt1/ATO as an anode catalyst, and an order of magnitude higher cell power is obtained...

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.

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.

Study of PtNi/C catalyst for direct ethanol fuel cell; Estudo do catalisador PtNi/C para celula a combustivel de etanol direto

Energy Technology Data Exchange (ETDEWEB)

Moraes, L.P.R. de; Silva, E.L. da; Amico, S.C.; Malfatti, C.F., E-mail: eticiaprm@gmail.com [Universidade Federal do Rio Grande do Sul (UFRGS), Porto Alegre, RS (Brazil)

2014-07-01

In this work, PtNi binary catalyst and pure platin catalyst were synthesized by the impregnation-reduction method, using Vulcan XC72R as support, for direct ethanol fuel cells. The composition and structure of the catalysts were analyzed by X-ray diffraction, the electrochemical behavior was evaluated by cyclic voltammetry and morphology of the catalysts was studied by high-resolution transmission electron microscopy. The results showed that the addition of Ni to Pt led to the contraction of the crystal lattice, increased the catalytic activity compared to pure Pt and initiated the electrooxidation of ethanol at lower potential. (author)

Palladium-Based Catalysts as Electrodes for Direct Methanol Fuel Cells: A Last Ten Years Review

Directory of Open Access Journals (Sweden)

Juan Carlos Calderón Gómez

2016-08-01

Full Text Available Platinum-based materials are accepted as the suitable electrocatalysts for anodes and cathodes in direct methanol fuel cells (DMFCs. Nonetheless, the increased demand and scarce world reserves of Pt, as well as some technical problems associated with its use, have motivated a wide research focused to design Pd-based catalysts, considering the similar properties between this metal and Pt. In this review, we present the most recent advancements about Pd-based catalysts, considering Pd, Pd alloys with different transition metals and non-carbon supported nanoparticles, as possible electrodes in DMFCs. In the case of the anode, different reported works have highlighted the capacity of these new materials for overcoming the CO poisoning and promote the oxidation of other intermediates generated during the methanol oxidation. Regarding the cathode, the studies have showed more positive onset potentials, as fundamental parameter for determining the mechanism of the oxygen reduction reaction (ORR and thus, making them able for achieving high efficiencies, with less production of hydrogen peroxide as collateral product. This revision suggests that it is possible to replace the conventional Pt catalysts by Pd-based materials, although several efforts must be made in order to improve their performance in DMFCs.

Enhanced activity and durability of platinum anode catalyst by the modification of cobalt phosphide for direct methanol fuel cells

International Nuclear Information System (INIS)

Li, Xiang; Wang, Hongjuan; Yu, Hao; Liu, Ziwu; Wang, Haihui; Peng, Feng

2015-01-01

Graphical abstract: A novel Pt/CoP/CNTs electrocatalyst with has been designed and prepared, which exhibits high activity and stability for methanol oxidation reaction. - Highlights: • Pt-cobalt phosphide catalyst supported on carbon nanotubes (Pt/CoP/CNTs) is designed. • Pt/CoP/CNTs exhibit high activity and stability for methanol oxidation reaction(MOR). • The effect of CoP content on electrocatalytic performances for MOR is studied. • CoP decreases the Pt particle size and increases the electrochemical surface areas. • The interaction between Pt and CoP is evidenced by X-ray photoelectron spectroscopy. - Abstract: In this study, carbon nanotubes (CNTs) supported Pt-cobalt phosphide (CoP) electrocatalyst (Pt/CoP/CNTs) is designed and prepared for methanol oxidation (MOR) for the first time. The modification of CoP decreases the Pt particle size significantly and increases the electrochemical surface areas due to the interaction between Pt and CoP, which is evidenced by transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. Among all these catalysts, Pt/4%CoP/CNTs catalyst exhibits the best MOR activity of 1600 mA mg −1 Pt , which is six times that of Pt/CNTs. Moreover, this catalyst also exhibits the higher onset current density and steady current density than the other Pt-based catalysts. The work provides a promising method to develop the highly active and stable Pt-based catalyst for direct methanol fuel cells.

Porous carbon as electrode material in direct ethanol fuel cells (DEFCs) synthesized by the direct carbonization of MOF-5

KAUST Repository

Khan, Inayatali

2014-01-12

Porous carbon (PC-900) was prepared by direct carbonization of porous metal-organic framework (MOF)-5 (Zn4O(bdc)3, bdc=1,4-benzenedicarboxylate) at 900 °C. The carbon material was deposited with PtM (M=Fe, Ni, Co, and Cu (20 %) metal loading) nanoparticles using the polyol reduction method, and catalysts PtM/PC-900 were designed for direct ethanol fuel cells (DEFCs). However, herein, we are reporting PtFe/PC-900 catalyst combination which has exhibited superior performance among other options. This catalyst was characterized by powder XRD, high-resolution transmission electron microscopy (HRTEM), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and selected area electron diffraction (SAED) technique. The electrocatalytic capability of the catalyst for ethanol electrooxidation was investigated using cyclic voltammetry and direct ethanol single cell testing. The results were compared with those of PtFe and Pt supported on Vulcan XC72 carbon catalysts (PFe/CX-72 and Pt/XC-72) prepared via the same method. It has been observed that the catalyst PtFe/PC-900 developed in this work showed an outstanding normalized activity per gram of Pt (6.8 mA/g Pt) and superior power density (121 mW/cm2 at 90 °C) compared to commercially available carbon-supported catalysts. © Springer-Verlag Berlin Heidelberg 2014.

Porous carbon as electrode material in direct ethanol fuel cells (DEFCs) synthesized by the direct carbonization of MOF-5

KAUST Repository

Khan, Inayatali; Badshah, Amin; Haider, Naghma; Ullah, Shafiq; Anjum, Dalaver H.; Nadeem, Muhammad Arif

2014-01-01

Porous carbon (PC-900) was prepared by direct carbonization of porous metal-organic framework (MOF)-5 (Zn4O(bdc)3, bdc=1,4-benzenedicarboxylate) at 900 °C. The carbon material was deposited with PtM (M=Fe, Ni, Co, and Cu (20 %) metal loading) nanoparticles using the polyol reduction method, and catalysts PtM/PC-900 were designed for direct ethanol fuel cells (DEFCs). However, herein, we are reporting PtFe/PC-900 catalyst combination which has exhibited superior performance among other options. This catalyst was characterized by powder XRD, high-resolution transmission electron microscopy (HRTEM), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and selected area electron diffraction (SAED) technique. The electrocatalytic capability of the catalyst for ethanol electrooxidation was investigated using cyclic voltammetry and direct ethanol single cell testing. The results were compared with those of PtFe and Pt supported on Vulcan XC72 carbon catalysts (PFe/CX-72 and Pt/XC-72) prepared via the same method. It has been observed that the catalyst PtFe/PC-900 developed in this work showed an outstanding normalized activity per gram of Pt (6.8 mA/g Pt) and superior power density (121 mW/cm2 at 90 °C) compared to commercially available carbon-supported catalysts. © Springer-Verlag Berlin Heidelberg 2014.

Visible-Light-Responsive Photocatalysis: Ag-Doped TiO2 Catalyst Development and Reactor Design Testing

Science.gov (United States)

Coutts, Janelle L.; Hintze, Paul E.; Meier, Anne; Shah, Malay G.; Devor, Robert W.; Surma, Jan M.; Maloney, Phillip R.; Bauer, Brint M.; Mazyck, David W.

2016-01-01

In recent years, the alteration of titanium dioxide to become visible-light-responsive (VLR) has been a major focus in the field of photocatalysis. Currently, bare titanium dioxide requires ultraviolet light for activation due to its band gap energy of 3.2 eV. Hg-vapor fluorescent light sources are used in photocatalytic oxidation (PCO) reactors to provide adequate levels of ultraviolet light for catalyst activation; these mercury-containing lamps, however, hinder the use of this PCO technology in a spaceflight environment due to concerns over crew Hg exposure. VLR-TiO2 would allow for use of ambient visible solar radiation or highly efficient visible wavelength LEDs, both of which would make PCO approaches more efficient, flexible, economical, and safe. Over the past three years, Kennedy Space Center has developed a VLR Ag-doped TiO2 catalyst with a band gap of 2.72 eV and promising photocatalytic activity. Catalyst immobilization techniques, including incorporation of the catalyst into a sorbent material, were examined. Extensive modeling of a reactor test bed mimicking air duct work with throughput similar to that seen on the International Space Station was completed to determine optimal reactor design. A bench-scale reactor with the novel catalyst and high-efficiency blue LEDs was challenged with several common volatile organic compounds (VOCs) found in ISS cabin air to evaluate the system's ability to perform high-throughput trace contaminant removal. The ultimate goal for this testing was to determine if the unit would be useful in pre-heat exchanger operations to lessen condensed VOCs in recovered water thus lowering the burden of VOC removal for water purification systems.

Direct Synthesis of Renewable Dodecanol and Dodecane with Methyl Isobutyl Ketone over Dual-Bed Catalyst Systems.

Science.gov (United States)

Sheng, Xueru; Li, Ning; Li, Guangyi; Wang, Wentao; Wang, Aiqin; Cong, Yu; Wang, Xiaodong; Zhang, Tao

2017-03-09

For the first time, we demonstrated two integrated processes for the direct synthesis of dodecanol or 2,4,8-trimethylnonane (a jet fuel range C 12 -branched alkane) using methyl isobutyl ketone (MIBK) that can be derived from lignocellulose. The reactions were carried out in dual-bed continuous flow reactors. In the first bed, MIBK was selectively converted to a mixture of C 12 alcohol and ketone. Over the Pd-modified magnesium- aluminium hydrotalcite (Pd-MgAl-HT) catalyst, a high total carbon yield (73.0 %) of C 12 oxygenates can be achieved under mild conditions. In the second bed, the C 12 oxygenates generated in the first bed were hydrogenated to dodecanol over a Ru/C catalyst or hydrodeoxygenated to 2,4,8-trimethylnonane over a Cu/SiO 2 catalyst. The as-obtained dodecanol can be used as feedstock in the production of sodium dodecylsulfate (SDS) and sodium dodecyl benzene sulfonate (SDBS), which are widely used as surfactants or detergents. The asobtained 2,4,8-trimethylnonane can be blended into conventional jet fuel without hydroisomerization. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts

Science.gov (United States)

Shan, Junjun; Li, Mengwei; Allard, Lawrence F.; Lee, Sungsik; Flytzani-Stephanopoulos, Maria

2017-11-01

An efficient and direct method of catalytic conversion of methane to liquid methanol and other oxygenates would be of considerable practical value. However, it remains an unsolved problem in catalysis, as typically it involves expensive or corrosive oxidants or reaction media that are not amenable to commercialization. Although methane can be directly converted to methanol using molecular oxygen under mild conditions in the gas phase, the process is either stoichiometric (and therefore requires a water extraction step) or is too slow and low-yielding to be practical. Methane could, in principle, also be transformed through direct oxidative carbonylation to acetic acid, which is commercially obtained through methane steam reforming, methanol synthesis, and subsequent methanol carbonylation on homogeneous catalysts. However, an effective catalyst for the direct carbonylation of methane to acetic acid, which might enable the economical small-scale utilization of natural gas that is currently flared or stranded, has not yet been reported. Here we show that mononuclear rhodium species, anchored on a zeolite or titanium dioxide support suspended in aqueous solution, catalyse the direct conversion of methane to methanol and acetic acid, using oxygen and carbon monoxide under mild conditions. We find that the two products form through independent pathways, which allows us to tune the conversion: three-hour-long batch-reactor tests conducted at 150 degrees Celsius, using either the zeolite-supported or the titanium-dioxide-supported catalyst, yield around 22,000 micromoles of acetic acid per gram of catalyst, or around 230 micromoles of methanol per gram of catalyst, respectively, with selectivities of 60-100 per cent. We anticipate that these unusually high activities, despite still being too low for commercial application, may guide the development of optimized catalysts and practical processes for the direct conversion of methane to methanol, acetic acid and other useful

Long term deactivation test of high dust SCR catalysts by straw co-firing

Energy Technology Data Exchange (ETDEWEB)

Weigang Lin; Degn Jensen, A.; Bjerkvig, J.

2009-12-15

The consequences of carbon dioxide induced global warming cause major concern worldwide. The consumption of energy produced with fossil fuels is the major factor that contributes to the global warming. Biomass is a renewable energy resource and has a nature of CO{sub 2} neutrality. Co-combustion of biomass in existing coal fired power plants can maintain high efficiency and reduce the emission of CO{sub 2} at same time. However, one of the problems faced by co-firing is deactivation of the SCR catalysts. Understanding of the mechanisms of deactivation of the catalyst elements at co-firing conditions is crucial for long term runs of the power plants. Twenty six SCR catalyst elements were exposed at two units (SSV3 and SSV4) in the Studstrup Power Plant for a long period. Both units co-fire coal and straw with a typical fraction of 8-10% straw on an energy basis during co-firing. SSV4 unit operated in co-firing mode most of the time; SSV3 unit co-fired straw half of the operating time. The main objective of this PSO-project is to gain knowledge of a long term influence on catalyst activity when co-firing straw in coal-fired power plants, thus, to improve the basis for operating the SCR-plants for NO{sub x}-reduction. The exposure time of the applied catalyst elements (HTAS and BASF) varied from approximately 5000 to 19000 hours in the power plant by exchanging the element two times. The activity of all elements was measured before and after exposure in a bench scale test rig at the Department of Chemical and Biochemical Engineering, Technical University of Denmark. The results show that the activity, estimated by exclusion of channel clogging of the elements, decreases gradually with the total exposure time. It appears that the exposure time under co-firing condition has little effect on the deactivation of the catalyst elements and no sharp decrease of the activity was observed. The average deactivation rate of the catalyst elements is 1.6 %/1000 hours. SEM

Optimization of catalyst system reaps economic benefits

International Nuclear Information System (INIS)

Le Roy, C.F.; Hanshaw, M.J.; Fischer, S.M.; Malik, T.; Kooiman, R.R.

1991-01-01

Champlin Refining and Chemicals Inc. is learning to optimize its catalyst systems for hydrotreating Venezuelan gas oils through a program of research, pilot plant testing, and commercial unit operation. The economic results of this project have been evaluated, and the benefits are most evident in improvements in product yields and qualities. The project has involved six commercial test runs, to date (Runs 10-15), with a seventh run planned. A summary of the different types of catalyst systems used in the test runs, and the catalyst philosophy that developed is given. Runs 10 and 11 used standard CoMo and NiMo catalysts for heavy gas oils hydrotreating. These catalysts had small pore sizes and suffered high deactivation rates because of metals contamination. When it was discovered that metals contamination was a problem, catalyst options were reviewed

Development and integration of a LabVIEW-based modular architecture for automated execution of electrochemical catalyst testing.

Science.gov (United States)

Topalov, Angel A; Katsounaros, Ioannis; Meier, Josef C; Klemm, Sebastian O; Mayrhofer, Karl J J

2011-11-01

This paper describes a system for performing electrochemical catalyst testing where all hardware components are controlled simultaneously using a single LabVIEW-based software application. The software that we developed can be operated in both manual mode for exploratory investigations and automatic mode for routine measurements, by using predefined execution procedures. The latter enables the execution of high-throughput or combinatorial investigations, which decrease substantially the time and cost for catalyst testing. The software was constructed using a modular architecture which simplifies the modification or extension of the system, depending on future needs. The system was tested by performing stability tests of commercial fuel cell electrocatalysts, and the advantages of the developed system are discussed. © 2011 American Institute of Physics

Investigation of Au-Pt/C electro-catalysts for oxygen reduction reaction

International Nuclear Information System (INIS)

Lin Rui; Zhang Haiyan; Zhao Tiantian; Cao Chunhui; Yang Daijun; Ma Jianxin

2012-01-01

Highlights: ► Au-Pt core shell catalyst. ► Seed-mediated growth method. ► Au-Pt (2:4)/C best activity toward ORR. ► Four-electron pathway in acid solution. ► Single cell performance. - Abstract: Carbon-supported Au-Pt core shell nano-structured catalysts were synthesized by the seed-mediated growth method. The nano-structured catalysts were characterized by UV–vis spectroscopy, X-ray photoelectron spectra (XPS) and transmission electron microscopy (TEM) techniques. The oxygen reduction reaction (ORR) activity of the Au-Pt/C was tested by means of linear sweep voltammetry (LSV) by employing rotating disk electrode (RDE). It revealed that Au-Pt (2:4)/C (atomic ratio) catalyst exhibited the best catalytic activity toward ORR. Au-Pt (2:4)/C proceeded by an approximately four-electron pathway in acid solution, through which molecular oxygen was directly reduced to water. The stability of Au-Pt (2:4)/C is tested by cyclic voltammetry for 500 cycles. The performance of the membrane electrode assembly (MEA) prepared by Au-Pt (2:4)/C as the cathode catalyst in a single proton exchange membrane fuel cell (PEMFC) generated a maximum power density of 479 mW cm −2 at 0.431 V using H 2 and O 2 at 80 °C.

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

International Nuclear Information System (INIS)

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

2012-01-01

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

Testing of the activity of a zeolite hydrocracking catalyst

Energy Technology Data Exchange (ETDEWEB)

Krichko, A A; Yulin, M K

1973-01-01

The activity of a catalyst having 3.5% of molybdena supported on the hydrogen form of sodium-Y zeolite remained constant during an 800 hour laboratory test carried out at 380/sup 0/C and 40 atm with an hourly space velocity of 1.0 and a hydrogen feed rate of 1000 l/l of feed on a 180 to 320/sup 0/C fraction obtained by hydrogenating a 35 : 65 mixture of coal and an atmospheric residuum boiling above 240/sup 0/C. The catalyst was first subjected to oxidative regeneration after 500 hours of high-temperature hydrogenation of aromatized extracts. A 56.2 to 61.9% conversion to a fraction boiling up to 180/sup 0/C was achieved with a 7.3 to 9.5% yield of gas consisting most of C/sub 3/-C/sub 4/ alkanes. The isobutene/n-butene ratio was 2.5 : 1 to 3.0 : 1. A 184 to 316/sup 0/C diesel fraction having a cetane number of 50.0 and a 46 to 177/sup 0/C gasoline fraction having a Motor octane number of 81.5 and a Research octane number of 91.0 were separated from the product.

Automotive Catalyst State Diagnosis Using Microwaves

Directory of Open Access Journals (Sweden)

Moos Ralf

2015-01-01

Full Text Available The state of catalysts plays a key role in automotive exhaust gas aftertreatment. The soot or ash loading of Diesel particulate filters, the oxygen loading degree in three-way catalysts, the amount of stored ammonia in SCR catalysts, or the NOx loading degree in NOx storage catalysts are important parameters that are today determined indirectly and in a model-based manner with gas sensors installed upstream and/or downstream of the catalysts. This contribution gives an overview on a novel approach to determine the catalyst state directly by a microwave-based technique. The method exploits the fact that the catalyst housing acts as a microwave cavity resonator. As “sensing” elements, one or two simple antennas are mounted inside the catalyst canning. The electrical properties of the catalyst device (ceramic honeycomb plus coating and storage material can be measured. Preferably, the resonance characteristics, e.g., the resonance frequencies, of selected cavity modes are observed. The information on the catalyst interior obtained in such a contactless manner is very well correlated with the catalyst state as will be demonstrated for different exhaust gas aftertreatment systems.

Engineering New Catalysts for In-Process Elimination of Tars

Energy Technology Data Exchange (ETDEWEB)

Felix, Larry G. [Gas Technology Inst., Des Plaines, IL (United States)

2012-09-30

The key objective of this project was to develop a new and more efficient methodology for engineering and economically producing optimized robust catalysts for the reduction or elimination of tars in biomass gasification. Whereas current catalyst technology typically disposes thin layers of catalytically-active material onto rigid supports via wet chemistry-based methods, this project investigated novel thermal methods for directly incorporating catalytically active materials onto robust supports as well as novel approaches for incorporating catalytically active materials on and/or within an otherwise inert refractory support material which is then subsequently formed and processed to create a catalytically-active material on all exposed surfaces. Specifically, the focus of this engineered catalyst development was on materials which were derived from, or otherwise related to, olivine-like minerals, due to the inherent attrition resistance and moderate catalytic properties exhibited by natural olivine when used in a fluidized bed biomass gasifier. Task 1 of this project successfully demonstrated the direct thermal impregnation of catalytically-active materials onto an olivine substrate, with the production of a Ni-olivine catalyst. Nickel and nickel oxide were thermally impregnated onto an olivine substrate and when reduced were shown to demonstrate improved catalytic activity over the baseline olivine material and equal the tar-decomposing performance of Ni-olivine catalysts prepared by conventional wet impregnation. Task 2 involved coordination with our subcontracted project partners to further develop and characterize catalyst formulations and to optimize activity and production methods. Within this task, several significant new materials were developed. NexTech Materials developed a sintered ceramic nickel-magnesium-silicate catalyst that demonstrated superb catalytic activity and high resistance to deactivation by H2S. Alfred University developed both supported

40 CFR 90.427 - Catalyst thermal stress resistance evaluation.

Science.gov (United States)

2010-07-01

... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Catalyst thermal stress resistance... Gaseous Exhaust Test Procedures § 90.427 Catalyst thermal stress resistance evaluation. (a) The purpose of... catalyst conversion efficiency for Phase 1 engines. The thermal stress is imposed on the test catalyst by...

The cycle use test of Pt based catalyst for the steam reforming of naphthalene / benzene as model tar compounds of biomass gasification

Energy Technology Data Exchange (ETDEWEB)

Furusawa, Takeshi; Saito, Katsuhiko; Sato, Masahide; Suzuki, Noboru [Utsunomiya Univ. (Japan). Graduate School of Engineering

2010-07-01

Although Pt/Al{sub 2}O{sub 3} catalyst showed high and stable activity (carbon conv. to gas: 90%) for steam reforming of naphthalene/benzene at 1073 K with S/C=3, this catalyst gradually lost its activity at 1023 K with S/C=3 due to deposition of carboneous species. Two kinds of regeneration treatment was conducted to enlongate the life time of Pt/Al{sub 2}O{sub 3} catalyst. Although regeneration treatment completely remove the carboneous species from catalyst, mild oxidation treatment led to decrease activity due to sintering of Pt particles. On the contrary, hydrogen treatment led to maintain activity until 5th cycle test. It was concluded from these obtained results that hydrogen treatment is suitable regeneration method during cycle test in the case of Pt/Al{sub 2}O{sub 3} catalyst. (orig.)

Plasma and catalyst for the oxidation of NOx

Science.gov (United States)

Jõgi, Indrek; Erme, Kalev; Levoll, Erik; Raud, Jüri; Stamate, Eugen

2018-03-01

Efficient exhaust gas cleaning from NO x (NO and NO2) by absorption and adsorption based methods requires the oxidation of NO. The application of non-thermal plasma is considered as a promising oxidation method but the oxidation of NO by direct plasma remains limited due to the back-reaction of NO2 to NO mediated by O radicals in plasma. Indirect NO oxidation by plasma produced ozone allows to circumvent the back-reaction and further oxidize NO2 to N2O5 but the slow reaction rate for the latter process limits the efficiency of this process. Present paper gives an overview of the role of metal-oxide catalysts in the improvement of oxidation efficiency for both direct and indirect plasma oxidation of NO x . The plasma produced active oxygen species (O, O3) were shown to play an important role in the reactions taking place on the catalyst surfaces while the exact mechanism and extent of the effect were different for direct and indirect oxidation. In the case of direct plasma oxidation, both short and long lifetime oxygen species could reach the catalyst and participate in the oxidation of NO to NO2. The back-reaction in the plasma phase remained still important factor and limited the effect of catalyst. In the case of indirect oxidation, only ozone could reach the catalyst surface and improve the oxidation of NO2 to N2O5. The effect of catalyst at different experimental conditions was quantitatively described with the aid of simple global chemical kinetic models derived for the NO x oxidation either by plasma or ozone. The models allowed to compare the effect of different catalysts and to analyze the limitations for the efficiency improvement by catalyst.

Catalysts for synthetic liquid fuels

Energy Technology Data Exchange (ETDEWEB)

Bruce, L.A.; Turney, T.W.

1987-12-01

Fischer-Tropsch catalysts have been designed, characterized and tested for the selective production of hydrocarbons suitable as synthetic liquid transport fuels from synthesis gas (i.e., by the reduction of carbon monoxide with hydrogen). It was found that hydrocarbons in the middle distillate range, or suitable for conversion to that range, could be produced over several of the new catalyst systems. The various catalysts examined included: (1) synthetic cobalt clays, mainly cobalt chlorites; (2) cobalt hydrotalcites; (3) ruthenium metal supported on rare earth oxides of high surface area; and (4) a novel promoted cobalt catalyst. Active and selective catalysts have been obtained, in each category. With the exception of the clays, reproducibility of catalyst performance has been good. Catalysts in groups 2 and 4 have exhibited very high activity, with long lifetimes and easy regeneration.

Based on a new support for synthesis of highly efficient palladium/hydroxyapatite catalyst for ethanol electrooxidation

International Nuclear Information System (INIS)

Cui, Qian; Chao, Shujun; Bai, Zhengyu; Yan, Huiying; Wang, Kui; Yang, Lin

2014-01-01

Based on a new support, hydroxyapatite (HAP), a facile and low–cost preparation of palladium/hydroxyapatite catalyst for ethanol electrooxidation is introduced in this paper through a solvothermal reaction without additives. HAP was employed as the catalyst support for its hydroxyl–rich surface in order to increase the stability and utilization ratio of catalyst. According to transmission electron microscopy (TEM), field emission scanning electron microscopy (FESEM) and X–ray diffraction (XRD) measurements, the as–prepared Pd nanoparticles with face–centered cubic crystal structure were evenly deposited on the surface of HAP. Cyclic voltammetry and chronoamperometry tests demonstrated that the Pd/HAP catalyst possessed a much higher current density (246 mA cm −2 ) than the Pd/C catalyst (109 mA cm −2 ) towards ethanol electrooxidation, and better stability as well. In the direct ethanol fuel cell (DEFC) test, Pd/HAP catalyst gives better performance than that with Pd/C in terms of both open-circuit voltage (OCV) and power density. These results indicate that the HAP is a better support and the catalyst developed in this study may be a better candidate for DEFCs. A possible mechanism consistent with the experimental is also proposed

Graphene-derived Fe/Co-N-C catalyst in direct methanol fuel cells: Effects of the methanol concentration and ionomer content on cell performance

Science.gov (United States)

Park, Jong Cheol; Choi, Chang Hyuck

2017-08-01

Non-precious metal catalysts (typically Fe(Co)-N-C catalysts) have been widely investigated for use as cost-effective cathode materials in low temperature fuel cells. Despite the high oxygen reduction activity and methanol-tolerance of graphene-based Fe(Co)-N-C catalysts in an acidic medium, their use in direct methanol fuel cells (DMFCs) has not yet been successfully implemented, and only a few studies have investigated this topic. Herein, we synthesized a nano-sized graphene-derived Fe/Co-N-C catalyst by physical ball-milling and a subsequent chemical modification of the graphene oxide. Twelve membrane-electrode-assemblies are fabricated with various cathode compositions to determine the effects of the methanol concentration, ionomer (i.e. Nafion) content, and catalyst loading on the DMFC performance. The results show that a graphene-based catalyst is capable of tolerating a highly-concentrated methanol feed up to 10.0 M. The optimized electrode composition has an ionomer content and catalyst loading of 66.7 wt% and 5.0 mg cm-2, respectively. The highest maximum power density is ca. 32 mW cm-2 with a relatively low PtRu content (2 mgPtRu cm-2). This study overcomes the drawbacks of conventional graphene-based electrodes using a nano-sized graphene-based catalyst and further shows the feasibility of their potential applications in DMFC systems.

Direct synthesis of iso-butane from synthesis gas or CO2 over CuZnZrAl/Pd-β hybrid catalyst

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Congming Li

2017-12-01

Full Text Available The effect of various factors on the catalytic performance of iso-butane formation over CuZnZrAl/Pd-β hybrid catalyst via synthesis gas or CO2 hydrogenation has been deeply investigated in this work. It was interesting to note that the iso-butane/n-butane ratio value was much higher than that of thermodynamic equilibrium (about 1/1, whose value was directly related to the reaction condition using this hybrid catalyst. In order to further clearly clarify this finding, various experimental reaction factors were selected to investigate the formation of iso-butane. The results revealed that increasing temperature, H2/COx, CO2/COx, and/or Pd loading possessed an inhibiting effect on the iso-butane yield. High selectivity of iso-butane could be achieved by increasing the reaction pressure, W/F and the weight ratio of CuZnZrAl methanol catalyst to Pd-β catalyst. It is also noted that the addition of water seriously suppressed the reaction activity, resulting in the low ratio of iso-butane/n-butane. A possible reaction route was elucidated based on the latest results. This might shed light on the development of a high efficient catalyst for iso-butane production from synthesis gas or CO2 hydrogenation. Keywords: Iso-butane, Synthesis gas, CO2, CuZnZrAl/Pd-β hybrid catalyst

Bifunctional cobalt F-T catalysts

Energy Technology Data Exchange (ETDEWEB)

Miller, J.G.; Coughlin, P.K.; Yang, C.L.; Rabo, J.A.

1986-03-01

Results on the catalytic screening of Fischer-Tropsch catalysts containing shape selective components are reported. Catalysts consist of promoted cobalt intimately contacted with Union Carbide molecular sieves and were tested using a Berty type internally recycled reactor. Methods of preparation, promoters and shape selective components were varied and aimed at improving catalyst performance. Catalysts were developed demonstrating high C/sub 5/ + yields with high olefin content and low methane production while maintaining stability under both low and high H/sub 2/:CO ratio conditions.

Effect of the thickness of the anode electrode catalyst layers on the performance in direct methanol fuel cells

Science.gov (United States)

Glass, Dean E.; Olah, George A.; Prakash, G. K. Surya

2017-06-01

For the large scale fuel cell manufacture, the catalyst loading and layer thickness are critical factors affecting the performance and cost of membrane electrode assemblies (MEAs). The influence of catalyst layer thicknesses at the anode of a PEM based direct methanol fuel cell (DMFC) has been investigated. Catalysts were applied with the drawdown method with varied thicknesses ranging from 1 mil to 8 mils (1 mil = 25.4 μm) with a Pt/Ru anode loading of 0.25 mg cm-2 to 2.0 mg cm-2. The MEAs with the thicker individual layers (8 mils and 4 mils) performed better overall compared to the those with the thinner layers (1 mil and painted). The peak power densities for the different loading levels followed an exponential decrease of Pt/Ru utilization at the higher loading levels. The highest power density achieved was 49 mW cm-2 with the 4 mil layers at 2.0 mg cm-2 catalyst loading whereas the highest normalized power density was 116 mW mg-1 with the 8 mil layers at 0.25 mg cm-2 loading. The 8 mil drawdowns displayed a 50% and 23% increase in normalized power density compared to the 1 mil drawdowns at 0.25 mg cm-2 and 0.5 mg cm-2 loadings, respectively.

SU-F-J-20: Commissioning and Acceptance Testing of the C-Rad CatalystHD Surface Imaging System

International Nuclear Information System (INIS)

Stanley, D; Rasmussen, K; Kirby, N; Papanikolaou, N; Gutierrez, A

2016-01-01

Introduction: With the increasing use of surface-based, nonionizing image-guided radiotherapy (IGRT) systems, a comprehensive set of clinical acceptance and commissioning procedures are needed to ensure correct functionality and proper clinical integration. Although TG-147 provides a specific set of parameters, measurement methodologies have yet to be described. The aim of this study was to provide a comprehensive overview of the commissioning and acceptance analysis performed for the C-Rad CatalystHD imaging system. Methods and Materials: Methodology for the commissioning and acceptance of the C-Rad CatalystHD imaging system was developed using commercially available clinical equipment. Following TG-147 guidelines, the following tests were performed: integration of peripheral equipment, system drift, static spatial reproducibility and localization accuracy, static end-to-end analysis, static rotational accuracy, dynamic spatial accuracy, dynamic temporal accuracy, dynamic radiation delivery and a comprehensive end-to-end analysis. Results: The field of view (FOV) of the CatalystHD was 105×109×83 cm3 in the lateral, longitudinal and vertical directions. For thermal equilibrium and system drift, a thermal drift of 1.0mm was noted. A 45 min warmup time is recommended if the system has been shut off an extended period of time (>24 hours) before the QA procedure to eliminate any thermal drift. Spatial reproducibility was found to be 0.05±0.03 mm using a rigid phantom. For the static localization accuracy, system agreement with couch shifts was within 0.1±0.1 mm and positioning agreement with kV-CBCT was 0.16±0.10 mm. For static rotational accuracy, system agreement with a high precision rotational stage (0.01 deg precision) was within 0.10±0.07 deg. Dynamic spatial and temporal localization accuracy was found to be within 0.2±0.1 mm. Conclusion: A comprehensive commissioning and acceptance study was performed using commercially available phantoms and in

Characterization of catalysts by scanning transmission electron microscopy

International Nuclear Information System (INIS)

Targos, W.M.; Bradley, S.A.

1989-01-01

The dedicated scanning transmission electron microscope (STEM) is an integral tool for characterizing catalysts because of its unique ability to image and analyze nanosized volumes. This information is valuable in optimizing catalyst formulations and determining causes for reduced catalyst performance. For many commercial catalysts direct correlations between structural features of metal crystallites and catalytic performance are not attainable. When these instances occur, determination of elemental distribution may be the only information available. In this paper the authors discuss some of the techniques employed and limitations associated with characterizing commercial catalysts

A proposed agglomerate model for oxygen reduction in the catalyst layer of proton exchange membrane fuel cells

International Nuclear Information System (INIS)

Zhang, Xiaoxian; Gao, Yuan; Ostadi, Hossein; Jiang, Kyle; Chen, Rui

2014-01-01

Highlights: • We developed a new agglomerate model to describe oxygen reduction reaction. • We showed how to calculate the model parameters from catalyst layer structure. • We verified the agglomerate model. - Abstract: Oxygen diffusion and reduction in the catalyst layer of PEM fuel cell is an important process in fuel cell modelling, but models able to link the reduction rate to catalyst-layer structure are lack; this paper makes such an effort. We first link the average reduction rate over the agglomerate within a catalyst layer to a probability that an oxygen molecule, which is initially on the agglomerate surface, will enter and remain in the agglomerate at any time in the absence of any electrochemical reaction. We then propose a method to directly calculate distribution function of this probability and apply it to two catalyst layers with contrasting structures. A formula is proposed to describe these calculated distribution functions, from which the agglomerate model is derived. The model has two parameters and both can be independently calculated from catalyst layer structures. We verify the model by first showing that it is an improvement and able to reproduce what the spherical model describes, and then testing it against the average oxygen reductions directly calculated from pore-scale simulations of oxygen diffusion and reaction in the two catalyst layers. The proposed model is simple, but significant as it links the average oxygen reduction to catalyst layer structures, and its two parameters can be directly calculated rather than by calibration

Catalytic hydrothermal liquefaction (HTL of biomass for bio-crude production using Ni/HZSM-5 catalysts

Directory of Open Access Journals (Sweden)

Shouyun Cheng

2017-04-01

Full Text Available Hydrothermal liquefaction (HTL is an effective method that can convert biomass into bio-crude, but direct use of bio-crude derived from biomass HTL remains a challenge due to the lower quality. In this study, bifunctional Ni/HZSM-5 catalysts and zinc hydrolysis were combined to produce upgraded bio-crude in an in-situ HTL process. The K2CO3 and HZSM-5 catalysts with different Ni loading ratios were tested. The effects of different catalysts on the yield and quality of bio-crude and gas were investigated. The results indicated that the catalysts improved bio-crude and gas yields, compared to pine sawdust liquefaction without catalyst. The catalysts reduced the contents of undesirable oxygenated compounds such as acids, ketones, phenols, alcohols and esters in bio-crude products while increased desirable hydrocarbons content. K2CO3 produced highest bio-crude yield and lowest solid residue yield among all catalysts. Compared to parent HZSM-5 catalyst, bifunctional Ni/HZSM-5 catalysts exhibited higher catalyst activity to improve quality of upgraded bio-crude due to its integration of cracking and hydrodeoxygenation reactions. 6%Ni/HZSM-5 catalyst produced the bio-crude with the highest hydrocarbons content at 11.02%. This catalyst can be a candidate for bio-crude production from biomass HTL.

Ag1 Pd1 Nanoparticles-Reduced Graphene Oxide as a Highly Efficient and Recyclable Catalyst for Direct Aryl C-H Olefination.

Science.gov (United States)

Hu, Qiyan; Liu, Xiaowang; Wang, Guoliang; Wang, Feifan; Li, Qian; Zhang, Wu

2017-12-14

The efficient and selective palladium-catalyzed activation of C-H bonds is of great importance for the construction of diverse bioactive molecules. Despite significant progress, the inability to recycle palladium catalysts and the need for additives impedes the practical applications of these reactions. Ag 1 Pd 1 nanoparticles-reduced graphene oxide (Ag 1 Pd 1 -rGO) was used as highly efficient and recyclable catalyst for the chelation-assisted ortho C-H bond olefination of amides with acrylates in good yields with a broad substrate scope. The catalyst can be recovered and reused at least 5 times without losing activity. A synergistic effect between the Ag and Pd atoms on the catalytic activity was found, and a plausible mechanism for the AgPd-rGO catalyzed C-H olefination is proposed. These findings suggest that the search for such Pd-based bimetallic alloy nanoparticles is a new method towards the development of superior recyclable catalysts for direct aryl C-H functionalization under mild conditions. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Report on the research achievements in the Sunshine Project in fiscal 1992. Studies on a direct gasification catalyst; 1992 nendo chokusetsu ekika shokubai ni kansuru kenkyu seika hokokusho

Energy Technology Data Exchange (ETDEWEB)

NONE

1993-10-01

This paper describes the research achievements in the Sunshine Project in fiscal 1992 in studies on a direct gasification catalyst. The paper summarizes the points where the catalyst research has reached to date. The catalyst surface effective for hydrogenation is the metal surface that can dissociate hydrogen. However, metals having large adsorption heat against hydrogen do not show the activity greatly because these metals are difficult of desorbing hydrogen having high dissociating activity. The coal liquefaction system has the surface oxidized by water content, wherein hydrogen dissociation cannot be expected, and sulfides are suitable. When a sulfide catalyst contacts hydrogen, the catalyst itself is desulfurized, producing H{sub 2}S and becomes a low-order sulfide. When atmospheric H{sub 2}S contacts this sulfide, it dissociates into HS and H, and this H behaves as active hydrogen. However, the liquefaction activity can be recognized even in a sulfuric acid type catalyst containing no sulfide whatsoever, wherein the H{sub 2}S partial pressure in the reaction system becomes extremely low. This fact means that the active hydrogen is not necessarily generated by the dissociation of H{sub 2}S. There is no other way but to think that hydrogen is dissociated directly without going through H{sub 2}S. If this is true, it provides a new guideline in developing and designing the future catalysts. (NEDO)

Improving the electrocatalytic properties of Pd-based catalyst for direct alcohol fuel cells: effect of solid solution.

Science.gov (United States)

Wen, Cuilian; Wei, Ying; Tang, Dian; Sa, Baisheng; Zhang, Teng; Chen, Changxin

2017-07-07

The tolerance of the electrode against the CO species absorbed upon the surface presents the biggest dilemma of the alcohol fuel cells. Here we report for the first time that the inclusion of (Zr, Ce)O 2 solid solution as the supporting material can significantly improve the anti-CO-poisoning as well as the activity of Pd/C catalyst for ethylene glycol electro-oxidation in KOH medium. In particular, the physical origin of the improved electrocatalytic properties has been unraveled by first principle calculations. The 3D stereoscopic Pd cluster on the surface of (Zr, Ce)O 2 solid solution leads to weaker Pd-C bonding and smaller CO desorption driving force. These results support that the Pd/ZrO 2 -CeO 2 /C composite catalyst could be used as a promising effective candidate for direct alcohol fuel cells application.

Novel metalloporphyrin catalysts for the oxidation of hydrocarbons

Energy Technology Data Exchange (ETDEWEB)

Showalter, M.C.; Nenoff, T.M.; Shelnutt, J.A.

1996-11-01

Work was done for developing biomimetic oxidation catalysts. Two classes of metalloporphyrin catalysts were studied. The first class of catalysts studied were a novel series of highly substituted metalloporphyrins, the fluorinated iron dodecaphenylporphyrins. These homogeneous metalloporphyrin catalysts were screened for activity as catalysts in the oxidation of hydrocarbons by dioxygen. Results are discussed with respect to catalyst structural features. The second type of catalysts studied were heterogeneous catalysts consisting of metalloporphyrins applied to inorganic supports. Preliminary catalytic testing results with these materials are presented.

High power passive μDMFC with low catalyst loading for small power generation

International Nuclear Information System (INIS)

Ahmad, M.M.; Kamarudin, S.K.; Daud, W.R.W.; Yaakub, Z.

2010-01-01

The main constraint for commercialization of micro direct methanol fuel cell (μDMFC) for small power generation is the performance of the fuel cell. In this study, a high power μDMFC with a power output of 56 mW and an active area of 4 cm 2 was successfully developed. The cell required low catalyst loading of 5 mg cm -2 and 0.5 mg cm -2 at the anode and cathode, respectively. Optimal design parameters for methanol concentration and catalyst loading were examined. Finally, long-term performance testing was performed and OCV curves are reported. The results obtained for this gives the highest power density at low catalyst loading as compare to other researchers in this area.

Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol

DEFF Research Database (Denmark)

Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank

2014-01-01

The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO 2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO...... 2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO 2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni......-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni 5 Ga 3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al 2 O 3 catalysts revealed the same or better methanol synthesis activity, as well as considerably...

Method of Heating a Foam-Based Catalyst Bed

Science.gov (United States)

Fortini, Arthur J.; Williams, Brian E.; McNeal, Shawn R.

2009-01-01

A method of heating a foam-based catalyst bed has been developed using silicon carbide as the catalyst support due to its readily accessible, high surface area that is oxidation-resistant and is electrically conductive. The foam support may be resistively heated by passing an electric current through it. This allows the catalyst bed to be heated directly, requiring less power to reach the desired temperature more quickly. Designed for heterogeneous catalysis, the method can be used by the petrochemical, chemical processing, and power-generating industries, as well as automotive catalytic converters. Catalyst beds must be heated to a light-off temperature before they catalyze the desired reactions. This typically is done by heating the assembly that contains the catalyst bed, which results in much of the power being wasted and/or lost to the surrounding environment. The catalyst bed is heated indirectly, thus requiring excessive power. With the electrically heated catalyst bed, virtually all of the power is used to heat the support, and only a small fraction is lost to the surroundings. Although the light-off temperature of most catalysts is only a few hundred degrees Celsius, the electrically heated foam is able to achieve temperatures of 1,200 C. Lower temperatures are achievable by supplying less electrical power to the foam. Furthermore, because of the foam s open-cell structure, the catalyst can be applied either directly to the foam ligaments or in the form of a catalyst- containing washcoat. This innovation would be very useful for heterogeneous catalysis where elevated temperatures are needed to drive the reaction.

Confined-interface-directed synthesis of Palladium single-atom catalysts on graphene/amorphous carbon

DEFF Research Database (Denmark)

Xi, Jiangbo; Sun, Hongyu; Zhang, Zheye

2018-01-01

The maximized atomic efficiency of supported catalysts is highly desired in heterogeneous catalysis. Therefore, the design and development of active, stable, and atomic metal-based catalysts remains a formidable challenge. To tackle these problems, it is necessary to investigate the interaction b...

ACTIVITY TEST AND REGENERATION OF NiMo/Z CATALYST FOR HYDROCRACKING OF WASTE PLASTIC FRACTION TO GASOLINE FRACTION

Directory of Open Access Journals (Sweden)

Rodiansono Rodiansono

2010-06-01

Full Text Available Activity test and regeneration of NiMo/active natural zeolite catalyst for hydrocracking of waste plastic fraction of polyprophylene (PP type have been carried out. The catalysts was prepared by loading Mo followed by Ni Metals onto the natural zeolite (Z sample, then calcined at 500oC, oxidized and reduced at 400oC under nitrogen, oxygen and hydrogen stream, respectively. The characterization of catalysts including spesific surface area, average pore radius, and total pore volume were performed by gas sorption analyzer, amount of total acid sites was determined by gas sorption method, and acid site strength was confirmed by IR spectroscopy. The hydrocracking process was carried out in a semi-flow reactor system at 360 oC and catalyst:feed ratio 0.5 under hydrogen stream (150 mL/hour. The feed was vaporized from the pyrolisis reactor into the hydrocracking reactor. A liquid product was collected and analyzed by gas chromatography (GC and gas chromatography-mass spectroscopy (GC-MS. The characterization results showed that spesific surface area, average pore radius, and total pore volume of the Z sample decreased after loading of the Ni and Mo metals. Amount of total acid sites of the NiMo/Z catalyst was higher than that of the Z sample. The activity of NiMo/Z catalyst decreased after several continously runs. Its regeneration produced the NiMo/Z reg catalyst with similar activity and selectivity to the fresh catalyst (NiMo/Z. The activity of catalysts at the optimum condition followed the order of NiMo/Z reg>NiMo/Z>Z (conversion of hydrocarbon C>12 and NiMo/Z reg>NiMo/Z>Z (total yield of gasoline fraction. The selectivity of catalysts for C7-C8 product followed the order of Z>NiMo/Z>NiMo/Z reg. Keywords: activity, polyprophylene, catalyst, gasoline fraction.

A genetically optimized kinetic model for ethanol electro-oxidation on Pt-based binary catalysts used in direct ethanol fuel cells

Science.gov (United States)

Sánchez-Monreal, Juan; García-Salaberri, Pablo A.; Vera, Marcos

2017-09-01

A one-dimensional model is proposed for the anode of a liquid-feed direct ethanol fuel cell. The complex kinetics of the ethanol electro-oxidation reaction is described using a multi-step reaction mechanism that considers free and adsorbed intermediate species on Pt-based binary catalysts. The adsorbed species are modeled using coverage factors to account for the blockage of the active reaction sites on the catalyst surface. The reaction rates are described by Butler-Volmer equations that are coupled to a one-dimensional mass transport model, which incorporates the effect of ethanol and acetaldehyde crossover. The proposed kinetic model circumvents the acetaldehyde bottleneck effect observed in previous studies by incorporating CH3CHOHads among the adsorbed intermediates. A multi-objetive genetic algorithm is used to determine the reaction constants using anode polarization and product selectivity data obtained from the literature. By adjusting the reaction constants using the methodology developed here, different catalyst layers could be modeled and their selectivities could be successfully reproduced.

Direct ethanol fuel cells with catalysed metal mesh anodes

International Nuclear Information System (INIS)

Chetty, Raghuram; Scott, Keith

2007-01-01

Platinum based binary and ternary catalysts prepared by thermal decomposition on titanium mesh were characterised and compared in terms of the electrochemical activity for ethanol oxidation. An enhancement in the catalytic activity was observed for the binary catalyst containing tin and ruthenium in their compositions with platinum. The catalysts were tested in single direct ethanol fuel cells and the result obtained with PtRu and PtSn showed that the mesh based electrodes show competitive performance in comparison to the conventional carbon based anodes

Pt-Ni and Pt-M-Ni (M = Ru, Sn Anode Catalysts for Low-Temperature Acidic Direct Alcohol Fuel Cells: A Review

Directory of Open Access Journals (Sweden)

Ermete Antolini

2017-01-01

Full Text Available In view of a possible use as anode materials in acidic direct alcohol fuel cells, the electro-catalytic activity of Pt-Ni and Pt-M-Ni (M = Ru, Sn catalysts for methanol and ethanol oxidation has been widely investigated. An overview of literature data regarding the effect of the addition of Ni to Pt and Pt-M on the methanol and ethanol oxidation activity in acid environment of the resulting binary and ternary Ni-containing Pt-based catalysts is presented, highlighting the effect of alloyed and non-alloyed nickel on the catalytic activity of these materials.

Catalyst in Basic Oleochemicals

Directory of Open Access Journals (Sweden)

Eva Suyenty

2007-10-01

Full Text Available Currently Indonesia is the world largest palm oil producer with production volume reaching 16 million tones per annum. The high crude oil and ethylene prices in the last 3 – 4 years contribute to the healthy demand growth for basic oleochemicals: fatty acids and fatty alcohols. Oleochemicals are starting to replace crude oil derived products in various applications. As widely practiced in petrochemical industry, catalyst plays a very important role in the production of basic oleochemicals. Catalytic reactions are abound in the production of oleochemicals: Nickel based catalysts are used in the hydrogenation of unsaturated fatty acids; sodium methylate catalyst in the transesterification of triglycerides; sulfonic based polystyrene resin catalyst in esterification of fatty acids; and copper chromite/copper zinc catalyst in the high pressure hydrogenation of methyl esters or fatty acids to produce fatty alcohols. To maintain long catalyst life, it is crucial to ensure the absence of catalyst poisons and inhibitors in the feed. The preparation methods of nickel and copper chromite catalysts are as follows: precipitation, filtration, drying, and calcinations. Sodium methylate is derived from direct reaction of sodium metal and methanol under inert gas. The sulfonic based polystyrene resin is derived from sulfonation of polystyrene crosslinked with di-vinyl-benzene. © 2007 BCREC UNDIP. All rights reserved.[Presented at Symposium and Congress of MKICS 2007, 18-19 April 2007, Semarang, Indonesia][How to Cite: E. Suyenty, H. Sentosa, M. Agustine, S. Anwar, A. Lie, E. Sutanto. (2007. Catalyst in Basic Oleochemicals. Bulletin of Chemical Reaction Engineering and Catalysis, 2 (2-3: 22-31.  doi:10.9767/bcrec.2.2-3.6.22-31][How to Link/DOI: http://dx.doi.org/10.9767/bcrec.2.2-3.6.22-31 || or local: http://ejournal.undip.ac.id/index.php/bcrec/article/view/6

Micelle-derived catalysts for extended Schulz-Flory

Energy Technology Data Exchange (ETDEWEB)

Abrevaya, H.

1986-01-01

The objective of this program is to develop a synthesis gas conversion catalyst with higher selectivity to liquid fuels, while maintaining catalytic activity and stability at least equivalent relative to state-of-the-art precipitated iron catalysts. During this quarter, the emphasis in the program has been the investigation of the hydrocarbon cutoff hypothesis with supported ruthenium catalysts. An alumina-supported catalyst with smaller than 20[Angstrom] ruthenium particles was tested under conditions of maximal water gas shift activity. During this test more than 90% of the water made in the Fischer-Tropsch synthesis reaction was converted to H[sub 2]. However, the extent of ruthenium metal agglomeration was not reduced. Accordingly, it was not possible to conclude whether hydrocarbon cutoff occurs with smaller than 20[Angstrom] ruthenium particles on [gamma]-alumina. A ruthenium catalyst prepared on Y-type zeolite had 20[Angstrom] or smaller ruthenium particles according to STEM examination and a 15[Angstrom] average ruthenium metal particle size according to EXAFS examination. The ruthenium metal particle size was stable during the test with this catalyst. The hydrocarbon product distribution was Anderson-Schulz-Flory with no cutoff up to a carbon number of 160. A well-dispersed titania-supported ruthenium catalyst is going to be evaluated during the next quarter in order to determine whether hydrocarbon cutoff occurs.

Performance Testing of Hydrodesulfurization Catalysts Using a Single-Pellet-String Reactor

NARCIS (Netherlands)

Moonen, Roel; Ras, Erik Jan; Harvey, Clare; Alles, Jeroen; Moulijn, J.A.

2017-01-01

Small-scale parallel trickle-bed reactors were used to evaluate the performance of a commercial hydrodesulfurization catalyst under industrially relevant conditions. Catalyst extrudates were loaded as a single string in reactor tubes. It is demonstrated that product sulfur levels and densities

Directing reaction pathways by catalyst active-site selection using self-assembled monolayers.

Science.gov (United States)

Pang, Simon H; Schoenbaum, Carolyn A; Schwartz, Daniel K; Medlin, J Will

2013-01-01

One key route for controlling reaction selectivity in heterogeneous catalysis is to prepare catalysts that exhibit only specific types of sites required for desired product formation. Here we show that alkanethiolate self-assembled monolayers with varying surface densities can be used to tune selectivity to desired hydrogenation and hydrodeoxygenation products during the reaction of furfural on supported palladium catalysts. Vibrational spectroscopic studies demonstrate that the selectivity improvement is achieved by controlling the availability of specific sites for the hydrogenation of furfural on supported palladium catalysts through the selection of an appropriate alkanethiolate. Increasing self-assembled monolayer density by controlling the steric bulk of the organic tail ligand restricts adsorption on terrace sites and dramatically increases selectivity to desired products furfuryl alcohol and methylfuran. This technique of active-site selection simultaneously serves both to enhance selectivity and provide insight into the reaction mechanism.

New catalysts for coal processing: Metal carbides and nitrides

Energy Technology Data Exchange (ETDEWEB)

S. Ted Oyama; David F. Cox

1999-12-03

The subject of this research project was to investigate the catalytic properties of a new class of materials, transition metal carbides and nitrides, for treatment of coal liquid and petroleum feedstocks. The main objectives were: (1) preparation of catalysts in unsupported and supported form; (2) characterization of the materials; (3) evaluation of their catalytic properties in HDS and HDN; (4) measurement of the surface properties; and (5) observation of adsorbed species. All of the objectives were substantially carried out and the results will be described in detail below. The catalysts were transition metal carbides and nitrides spanning Groups 4--6 in the Periodic Table. They were chosen for study because initial work had shown they were promising materials for hydrotreating. The basic strategy was first to prepare the materials in unsupported form to identify the most promising catalyst, and then to synthesize a supported form of the material. Already work had been carried out on the synthesis of the Group VI compounds Mo{sub 2}C, Mo{sub 2}N, and WC, and new methods were developed for the Group V compounds VC and NbC. All the catalysts were then evaluated in a hydrotreating test at realistic conditions. It was found that the most active catalyst was Mo{sub 2}C, and further investigations of the material were carried out in supported form. A new technique was employed for the study of the bulk and surface properties of the catalysts, near edge x-ray absorption spectroscopy (NEXAFS), that fingerprinted the electronic structure of the materials. Finally, two new research direction were explored. Bimetallic alloys formed between two transition metals were prepared, resulting in catalysts having even higher activity than Mo{sub 2}C. The performance of the catalysts in hydrodechloration was also investigated.

Determination of the NOx Loading of an Automotive Lean NOx Trap by Directly Monitoring the Electrical Properties of the Catalyst Material Itself

Directory of Open Access Journals (Sweden)

Ralf Moos

2011-08-01

Full Text Available Recently, it has been shown that the degree of loading of several types of automotive exhaust aftertreatment devices can be directly monitored in situ and in a contactless way by a microwave-based method. The goal of this study was to clarify whether this method can also be applied to NOx storage and reduction catalysts (lean NOx traps in order to obtain further knowledge about the reactions occurring in the catalyst and to compare the results with those obtained by wirebound NOx loading sensors. It is shown that both methods are able to detect the different catalyst loading states. However, the sensitivity of the microwave-based method turned out to be small compared to that previously observed for other exhaust aftertreatment devices. This may limit the practical applicability of the microwave-based NOx loading detection in lean NOx traps.

Direct transformation of xylan-type hemicelluloses to furfural via SnCl₄ catalysts in aqueous and biphasic systems.

Science.gov (United States)

Wang, Wenju; Ren, Junli; Li, Huiling; Deng, Aojie; Sun, Runcang

2015-05-01

Direct catalytic transformation of xylan-type hemicelluloses to furfural in the aqueous system and the biphasic system were comparatively investigated under mild conditions. Screening of several promising chlorides for conversion of beech xylan in the aqueous system revealed the Lewis acid SnCl4 was the most effective catalyst. Comparing to the single aqueous system, the bio-based 2-methyltetrahydrofuran (2-MTHF)/H2O biphasic system was more conducive to the synthesis of furfural, in which the highest furfural yield of 78.1% was achieved by using SnCl4 as catalysts under the optimized reaction conditions (150°C, 120 min). Additionally, the influences of xylan-type hemicelluloses with different chemical and structural features from beech, corncob and bagasse on the furfural production were studied. It was found that furfural yield to some extent was determined by the xylose content in hemicelluloses and also had relationships with the molecular weight of hemicelluloses and the degree of crystallization. Copyright © 2015 Elsevier Ltd. All rights reserved.

CATALYSTS NHI Thermochemical Systems FY 2009 Year-End Report

International Nuclear Information System (INIS)

Ginosar, Daniel M.

2009-01-01

Fiscal Year 2009 work in the Catalysts project focused on advanced catalysts for the decomposition of sulfuric acid, a reaction common to both the Sulfur-Iodine (S-I) cycle and the Hybrid Sulfur cycle. Prior years effort in this project has found that although platinum supported on titanium oxide will be an acceptable catalyst for sulfuric acid decomposition in the integrated laboratory scale (ILS) project, the material has short comings, including significant cost and high deactivation rates due to sintering and platinum evaporation. For pilot and larger scale systems, the catalyst stability needs to be improved significantly. In Fiscal Year 2008 it was found that at atmospheric pressure, deactivation rates of a 1 wt% platinum catalyst could be reduced by 300% by adding either 0.3 wt% iridium (Ir) or 0.3 wt% ruthenium (Ru) to the catalyst. In Fiscal Year 2009, work focused on examining the platinum group metal catalysts activity and stability at elevated pressures. In addition, simple and complex metal oxides are known to catalyze the sulfuric acid decomposition reaction. These metal oxides could offer activities comparable to platinum but at significantly reduced cost. Thus a second focus for Fiscal Year 2009 was to explore metal oxide catalysts for the sulfuric acid decomposition reaction. In Fiscal Year 2007 several commercial activated carbons had been identified for the HI decomposition reaction; a reaction specific to the S-I cycle. Those materials should be acceptable for the pilot scale project. The activated carbon catalysts have some disadvantages including low activity at the lower range of reactor operating temperature (350 to 400 C) and a propensity to generate carbon monoxide in the presence of water that could contaminate the hydrogen product, but due to limited funding, this area had low priority in Fiscal Year 2009. Fiscal Year 2009 catalyst work included five tasks: development, and testing of stabilized platinum based H2SO4 catalysts

ENVIRONMENTAL TECHNOLOGY VERIFICATION, TEST REPORT OF MOBILE SOURCE EMISSIONS CONTROL DEVICES/CLEAN DIESEL TECHNOLOGIES FUEL BORNE CATALYST WITH CLEANAIR SYSTEM'S DIESEL OXIDATION CATALYST

Science.gov (United States)

The Environmental Technology Verification report discusses the technology and performance of the Fuel-Borne Catalyst with CleanAir System's Diesel Oxidation Catalyst manufactured by Clean Diesel Technologies, Inc. The technology is a fuel-borne catalyst used in ultra low sulfur d...

Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst

Science.gov (United States)

Chung, Hoon T.; Cullen, David A.; Higgins, Drew; Sneed, Brian T.; Holby, Edward F.; More, Karren L.; Zelenay, Piotr

2017-08-01

Platinum group metal-free (PGM-free) metal-nitrogen-carbon catalysts have emerged as a promising alternative to their costly platinum (Pt)-based counterparts in polymer electrolyte fuel cells (PEFCs) but still face some major challenges, including (i) the identification of the most relevant catalytic site for the oxygen reduction reaction (ORR) and (ii) demonstration of competitive PEFC performance under automotive-application conditions in the hydrogen (H2)-air fuel cell. Herein, we demonstrate H2-air performance gains achieved with an iron-nitrogen-carbon catalyst synthesized with two nitrogen precursors that developed hierarchical porosity. Current densities recorded in the kinetic region of cathode operation, at fuel cell voltages greater than ~0.75 V, were the same as those obtained with a Pt cathode at a loading of 0.1 milligram of Pt per centimeter squared. The proposed catalytic active site, carbon-embedded nitrogen-coordinated iron (FeN4), was directly visualized with aberration-corrected scanning transmission electron microscopy, and the contributions of these active sites associated with specific lattice-level carbon structures were explored computationally.

Catalyst deterioration over the lifetime of small utility engines.

Science.gov (United States)

Doll, Nicholas J; Reisel, John R

2007-10-01

In this paper, the deterioration of catalysts in small, four-stroke, spark-ignition engines is described. The laboratory testing performed followed a proven test method that mimics the lifetime of a small air-cooled utility engine operating under normal field conditions. The engines used were single-cylinder, 6.5-hp, side-valve engines. These engines have a nominal 125-hr lifetime. The effectiveness of the catalysts was determined by testing exhaust emissions before and after the catalyst to determine the catalyst's efficiency. This was done several times during the lifetime of the engines to determine the deterioration in the performance of the catalysts at lowering pollutant emissions. Additional testing was performed on the catalysts to determine wear patterns, contamination, and recoverable activity. The results indicate that considerable catalyst deterioration is occurring over the lifetime of the engine. The results reveal that soot buildup, poisons, and active surface loss appear to be the contributing factors to the deterioration. These results were determined after analyzing the exhaust emissions data, scanning electron microscope results analysis, and the impact of regeneration attempts. An ANOVA statistical analysis was performed, and it was determined that the emissions are also impacted, to some degree, by time and the engine itself.

A novel catalyst layer structure based surface-patterned Nafion® membrane for high-performance direct methanol fuel cell

DEFF Research Database (Denmark)

Chen, Ming; Wang, Meng; Ding, Xianan

2018-01-01

.5% respectively, compared with the conventional catalyst layer. Performance improvement is attributed to the fact that the novel catalyst layer structure optimizes the electrolyte membrane/catalyst layer and gas diffusion layer/catalyst layer interfacial structure, which increases the electrochemical reaction......Conventional catalyst layer with a smooth surface exists the larger area of“catalytic dead zone” and reduces the utilization of catalyst. Based on this, a novel catalyst layer structure based surface-patterned Nafion® membrane was designed to achieve more efficient electrochemical reaction...... to prepare the novel catalyst layer, and the effect of pressure on the performance of MEA was investigated. The results suggested that the peak power density of DMFC with optimal novel catalyst layer structure increased by 28.84%, the charge transfer resistances of anode and cathode reduced by 28.8% and 26...

Influence of ionizing radiation on the catalytic properties of oxide catalysts tested by hydrogen peroxide decomposition

International Nuclear Information System (INIS)

Mucka, V.

1987-01-01

Results of a study of some physical and catalytic properties of different oxide catalysts as affected by ionizing radiation (γ, n, e - ) and tested by the decomposition of hydrogen peroxide in aqueous solution are presented in this paper. The oxidation state of the active component present on the catalyst surface was found to be one of the most sensitive properties to the ionizing radiation. Changes of this state induced by γ-irradiation were found to be positive in most cases; electron pre-irradiation of the oxides leads, as a rule, to negative effects and the effects of neutron irradiation may be positive or negative. On the other hand, changes in the catalytic activity of the oxides after γ-or electron-irradiation seem to be mostly negative and positive, respectively; the effects of fast neutrons seem to vary here. Neither quantitative or qualitative correlation was found between the radiation-induced changes in these two quantities. The results give evidence that ionizing radiation principally affects the surface concentration of the catalytic sites. Both the character and magnitude of the changes in surface oxidation abilities and in catalytic activities of the oxide catalysts seem to be dependent upon the actual state of the catalyst surface. (author)

Development of a Catalyst/Sorbent for Methane Reforming

Energy Technology Data Exchange (ETDEWEB)

B.H. Shans; T.D. Wheelock; Justinus Satrio; Karl Albrecht; Tanya Harris Janine Keeley; Ben Silva; Aaron Shell; Molly Lohry; Zachary Beversdorf

2008-12-31

conditions tested, the CH{sub 4} conversion was large (>80%) and nearly equal to the predicted thermodynamic equilibrium level as long as CO{sub 2} was being rapidly absorbed. Similar results were obtained with both shell material additives. Limited lifecycle tests of the pellets also produced similar results that were not affected by the choice of additive. However, during each lifecycle test the period during which CO{sub 2} was rapidly absorbed declined from cycle to cycle which directly affected the corresponding period when CH{sub 4} was reformed rapidly. Therefore, the results showed a continuing need for improving the lifecycle performance of the sorbent. Core-in-shell pellets with the improved shell materials were also utilized for conducting the water gas shift reaction in a single step. Three different catalyst formulations were tested. The best results were achieved with a Ni catalyst, which proved capable of catalyzing the reaction whether CO{sub 2} was being absorbed or not. The calcined alumina shell material by itself also proved to be a very good catalyst for the reaction as long as CO{sub 2} was being fully absorbed by the core material. However, neither the alumina nor a third formulation containing Fe{sub 2}O{sub 3} were good catalysts for the reaction when CO{sub 2} was not absorbed by the core material. Furthermore, the Fe{sub 2}O{sub 3}-containing catalyst was not as good as the other two catalysts when CO{sub 2} was being absorbed.

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.

Flame spray deposition of porous catalysts on surfaces and in microsystems

DEFF Research Database (Denmark)

Thybo, Susanne; Jensen, Søren; Johansen, Johnny

2004-01-01

Flame spray synthesis is investigated as a method for one step synthesis and deposition of porous catalysts onto surfaces and into microreactors. Using a standard photolithographic lift-off process, catalyst can be deposited on flat surfaces in patterns with sub-millimeter feature sizes....... With shadow masks, porous catalyst layers can be deposited selectively into microchannels. Using Au/TiO$_2$ as test catalyst and CO-oxidation as test reaction, it is found that the apparent activation energy of the deposited catalyst is similar to what is normally seen for supported gold catalysts...

Inhibition of Microbial Growth by Fatty Amine Catalysts from Polyurethane Foam Test Tube Plugs

Science.gov (United States)

Bach, John A.; Wnuk, Richard J.; Martin, Delano G.

1975-01-01

When polyurethane foam test tube plugs are autoclaved, they release volatile fatty amines that inhibit the growth of some microorganisms. The chemical structures of these amines were determined by the use of a gas chromatographmass spectrometer. They are catalysts used to produce the foam. The problem of contaminating growth media with toxic substances released from polymeric materials is discussed. PMID:1096816

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

Synthesis of Pd₃Co₁@Pt/C core-shell catalysts for methanol-tolerant cathodes of direct methanol fuel cells.

Science.gov (United States)

Aricò, Antonino S; Stassi, Alessandro; D'Urso, Claudia; Sebastián, David; Baglio, Vincenzo

2014-08-18

A composite Pd-based electrocatalyst consisting of a surface layer of Pt (5 wt.%) supported on a core Pd3Co1 alloy (95 wt.%) and dispersed as nanoparticles on a carbon black support (50 wt.% metal content) was prepared by using a sulphite-complex route. The structure, composition, morphology, and surface properties of the catalyst were investigated by XRD, XRF, TEM, XPS and low-energy ion scattering spectroscopy (LE-ISS). The catalyst showed an enrichment of Pt on the surface and a smaller content of Co in the outermost layers. These characteristics allow a decrease the Pt content in direct methanol fuel cell cathode electrodes (from 1 to 0.06 mg cm(-2)) without significant decay in performance, due also to a better tolerance to methanol permeated through the polymer electrolyte membrane. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Preparation and characterization of anode catalysts for the direct alcohol fuel cells (DAFC): methanol and ethanol

CSIR Research Space (South Africa)

Modibedi, M

2007-11-01

Full Text Available and M2 precursor solutions followed by reduction of the precursors. Catalysts prepared were: Pt-M1-M2/C (M1=Sn or Ru, M2= Ir). Phosphorus was deposited on these catalysts and their electrochemical activities were compared. The prepared catalysts were...

DEVELOPMENT OF PRECIPITATED IRON FISCHER-TROPSCH CATALYSTS

International Nuclear Information System (INIS)

Bukur, Dragomir B.; Lang, X.; Chokkaram, S.; Nowicki, L.; Wei, G.; Ding, Y.; Reddy, B.; Xiao, S.

1999-01-01

Despite the current worldwide oil glut, the US will ultimately require large-scale production of liquid (transportation) fuels from coal. Slurry phase Fischer-Tropsch (F-T) technology, with its versatile product slate, may be expected to play a major role in production of transportation fuels via indirect coal liquefaction. Some of the F-T catalysts synthesized and tested at Texas A and M University under DOE Contract No. DE-AC22-89PC89868 were more active than any other known catalysts developed for maximizing production of high molecular weight hydrocarbons (waxes). The objectives of the present contract were to demonstrate repeatability of catalyst performance and reproducibility of preparation procedures of two of these catalysts on a laboratory scale. Improvements in the catalyst performance were attempted through the use of: (a) higher reaction pressure and gas space velocity to maximize the reactor productivity; (b) modifications in catalyst preparation steps; and (c) different pretreatment procedures. Repeatability of catalyst performance and reproducibility of catalyst synthesis procedure have been successfully demonstrated in stirred tank slurry reactor tests. Reactor space-time-yield was increased up to 48% by increasing reaction pressure from 1.48 MPa to 2.17 MPa, while maintaining the gas contact time and synthesis gas conversion at a constant value. Use of calcination temperatures above 300 C, additional CaO promoter, and/or potassium silicate as the source of potassium promoter, instead of potassium bicarbonate, did not result in improved catalyst performance. By using different catalyst activation procedures they were able to increase substantially the catalyst activity, while maintaining low methane and gaseous hydrocarbon selectivities. Catalyst productivity in runs SA-0946 and SA-2186 was 0.71 and 0.86 gHC/g-Fe/h, respectively, and this represents 45-75% improvement in productivity relative to that achieved in Rheinpreussen's demonstration plant

Oxidation catalyst

Science.gov (United States)

Ceyer, Sylvia T.; Lahr, David L.

2010-11-09

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

Bimetallic catalysts for continuous catalytic wet air oxidation of phenol.

Science.gov (United States)

Fortuny, A; Bengoa, C; Font, J; Fabregat, A

1999-01-29

Catalytic wet oxidation has proved to be effective at eliminating hazardous organic compounds, such as phenol, from waste waters. However, the lack of active long-life oxidation catalysts which can perform in aqueous phase is its main drawback. This study explores the ability of bimetallic supported catalysts to oxidize aqueous phenol solutions using air as oxidant. Combinations of 2% of CoO, Fe2O3, MnO or ZnO with 10% CuO were supported on gamma-alumina by pore filling, calcined and later tested. The oxidation was carried out in a packed bed reactor operating in trickle flow regime at 140 degrees C and 900 kPa of oxygen partial pressure. Lifetime tests were conducted for 8 days. The pH of the feed solution was also varied. The results show that all the catalysts tested undergo severe deactivation during the first 2 days of operation. Later, the catalysts present steady activity until the end of the test. The highest residual phenol conversion was obtained for the ZnO-CuO, which was significantly higher than that obtained with the 10% CuO catalyst used as reference. The catalyst deactivation is related to the dissolution of the metal oxides from the catalyst surface due to the acidic reaction conditions. Generally, the performance of the catalysts was better when the pH of the feed solution was increased.

Screening of Catalysts for Hydrodeoxygenation of Phenol as Model Compound for Bio-oil

DEFF Research Database (Denmark)

Mortensen, Peter Mølgaard; Grunwaldt, Jan-Dierk; Jensen, Peter Arendt

2013-01-01

Four groups of catalysts have been tested for hydrodeoxygenation (HDO) of phenol as a model compound of bio-oil, including: oxide catalysts, methanol synthesis catalysts, reduced noble metal catalysts, and reduced non-noble metal catalysts. In total 23 different catalysts were tested at 100 bar H2...... and 275 °C in a batch reactor. The experiments showed that none of the tested oxides and methanol synthesis catalysts had any significant activity for phenol HDO at the given conditions, which were linked to their inability to hydrogenate the phenol. HDO of phenol over reduced metal catalysts could...... on a carbon support, but more active than the carbon supported noble metal catalysts when supported on ZrO2. This observation indicates that the nickel based catalysts require a metal oxide as carrier on which the activation of the phenol for the hydrogenation can take place through heterolytic dissociation...

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

Directory of Open Access Journals (Sweden)

Zhou Kai

2010-01-01

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

An optimization study of PtSn/C catalysts applied to direct ethanol fuel cell: Effect of the preparation method on the electrocatalytic activity of the catalysts

Science.gov (United States)

Almeida, T. S.; Palma, L. M.; Leonello, P. H.; Morais, C.; Kokoh, K. B.; De Andrade, A. R.

2012-10-01

The aim of this work was to perform a systematic study of the parameters that can influence the composition, morphology, and catalytic activity of PtSn/C nanoparticles and compare two different methods of nanocatalyst preparation, namely microwave-assisted heating (MW) and thermal decomposition of polymeric precursors (DPP). An investigation of the effects of the reducing and stabilizing agents on the catalytic activity and morphology of Pt75Sn25/C catalysts prepared by microwave-assisted heating was undertaken for optimization purposes. The effect of short-chain alcohols such as ethanol, ethylene glycol, and propylene glycol as reducing agents was evaluated, and the use of sodium acetate and citric acid as stabilizing agents for the MW procedure was examined. Catalysts obtained from propylene glycol displayed higher catalytic activity compared with catalysts prepared in ethylene glycol. Introduction of sodium acetate enhanced the catalytic activity, but this beneficial effect was observed until a critical acetate concentration was reached. Optimization of the MW synthesis allowed for the preparation of highly dispersed catalysts with average sizes lying between 2.0 and 5.0 nm. Comparison of the best catalyst prepared by MW with a catalyst of similar composition prepared by the polymeric precursors method showed that the catalytic activity of the material can be improved when a proper condition for catalyst preparation is achieved.

An XPS [x-ray photoelectron spectroscopy] study of the sulfidation-regeneration cycle of a hydroprocessing catalyst

Energy Technology Data Exchange (ETDEWEB)

Shang, D.Y.; Adnot, A.; Kaliaguine, S. (Laval Univ., Ste-Foy, PQ (Canada)); Chmielowiec, J. (Petro Canada Products Co., Mississauga, ON (Canada))

1993-10-01

The formation of sulfates in an industrial Ni-W hydroprocessing (HP) catalyst was investigated by x-ray photoelectron spectroscopy (XPS). A small fluidized bed test unit with on-line sampling device was constructed to simulate industrial sulfidation and oxyregeneration processes of HP catalysts. The results obtained show that the sulfates observed on the surface of sulfided catalysts are not formed during the sulfidation process. Two oxidation processes seem to be responsible for the formation of sulfates: one happens when the catalyst is exposed to air before it is properly cooled and the other is a slow conversion at ambient temperature. The two different processes might be associated to different sulfidic species formed during the sulfidation processes, with the sulfides in the bulk of catalyst particles being more easily oxidized than the ones on the external surface of the catalyst particles. The sulfate formed during the air oxidation of sulfided catalysts, as well as that after oxyregeneration, is not aluminum sulfate but nickel sulfate in both cases. XPS results also indicate that oxygenates in the feedstock are not directly involved in the sulfate formation. 18 refs., 9 figs., 6 tabs.

Noble metal catalysts in the production of biofuels

Energy Technology Data Exchange (ETDEWEB)

Gutierrez, A.

2013-11-01

The energy demand is increasing in the world together with the need to ensure energy security and the desire to decrease greenhouse gas emissions. While several renewable alternatives are available for the production of electricity, e.g. solar energy, wind power, and hydrogen, biomass is the only renewable source that can meet the demand for carbon-based liquid fuels and chemicals. The technology applied in the conversion of biomass depends on the type and complexity of the biomass, and the desired fuel. Hydrogen and hydrogen-rich mixtures (synthesis gas) are promising energy sources as they are more efficient and cleaner than existing fuels, especially when they are used in fuel cells. Hydrotreatment is a catalytic process that can be used in the conversion of biomass or biomass-derived liquids into fuels. In autothermal reforming (ATR), catalysts are used in the production of hydrogen-rich mixtures from conventional fuels or bio-fuels. The different nature of biomass and biomass-derived liquids and mineral oil makes the use of catalysts developed for the petroleum industry challenging. This requires the improvement of available catalysts and the development of new ones. To overcome the limitations of conventional hydrotreatment and ATR catalysts, zirconia-supported mono- and bimetallic rhodium, palladium, and platinum catalysts were developed and tested in the upgrading of model compounds for wood-based pyrolysis oil and in the production of hydrogen, using model compounds for gasoline and diesel. Catalysts were also tested in the ATR of ethanol. For comparative purposes commercial catalysts were tested and the results obtained with model compounds were compared with those obtained with real feedstocks (hydrotreatmet tests with wood-based pyrolysis oil and ATR tests with NExBTL renewable diesel). Noble metal catalysts were active and selective in the hydrotreatment of guaiacol used as the model compound for the lignin fraction of wood-based pyrolysis oil and wood

ADVANCED BYPRODUCT RECOVERY: DIRECT CATALYTIC REDUCTION OF SO2 TO ELEMENTAL SULFUR

Energy Technology Data Exchange (ETDEWEB)

Robert S. Weber

1999-05-01

Arthur D. Little, Inc., together with its commercialization partner, Engelhard Corporation, and its university partner Tufts, investigated a single-step process for direct, catalytic reduction of sulfur dioxide from regenerable flue gas desulfurization processes to the more valuable elemental sulfur by-product. This development built on recently demonstrated SO{sub 2}-reduction catalyst performance at Tufts University on a DOE-sponsored program and is, in principle, applicable to processing of regenerator off-gases from all regenerable SO{sub 2}-control processes. In this program, laboratory-scale catalyst optimization work at Tufts was combined with supported catalyst formulation work at Engelhard, bench-scale supported catalyst testing at Arthur D. Little and market assessments, also by Arthur D. Little. Objectives included identification and performance evaluation of a catalyst which is robust and flexible with regard to choice of reducing gas. The catalyst formulation was improved significantly over the course of this work owing to the identification of a number of underlying phenomena that tended to reduce catalyst selectivity. The most promising catalysts discovered in the bench-scale tests at Tufts were transformed into monolith-supported catalysts at Engelhard. These catalyst samples were tested at larger scale at Arthur D. Little, where the laboratory-scale results were confirmed, namely that the catalysts do effectively reduce sulfur dioxide to elemental sulfur when operated under appropriate levels of conversion and in conditions that do not contain too much water or hydrogen. Ways to overcome those limitations were suggested by the laboratory results. Nonetheless, at the end of Phase I, the catalysts did not exhibit the very stringent levels of activity or selectivity that would have permitted ready scale-up to pilot or commercial operation. Therefore, we chose not to pursue Phase II of this work which would have included further bench-scale testing

Diamond nanoparticles as a support for Pt and PtRu catalysts for direct methanol fuel cells.

Science.gov (United States)

La-Torre-Riveros, Lyda; Guzman-Blas, Rolando; Méndez-Torres, Adrián E; Prelas, Mark; Tryk, Donald A; Cabrera, Carlos R

2012-02-01

Diamond in nanoparticle form is a promising material that can be used as a robust and chemically stable catalyst support in fuel cells. It has been studied and characterized physically and electrochemically, in its thin film and powder forms, as reported in the literature. In the present work, the electrochemical properties of undoped and boron-doped diamond nanoparticle electrodes, fabricated using the ink-paste method, were investigated. Methanol oxidation experiments were carried out in both half-cell and full fuel cell modes. Platinum and ruthenium nanoparticles were chemically deposited on undoped and boron doped diamond nanoparticles through the use of NaBH(4) as reducing agent and sodium dodecyl benzene sulfonate (SDBS) as a surfactant. Before and after the reduction process, samples were characterized by electron microscopy and spectroscopic techniques. The ink-paste method was also used to prepare the membrane electrode assembly with Pt and Pt-Ru modified undoped and boron-doped diamond nanoparticle catalytic systems, to perform the electrochemical experiments in a direct methanol fuel cell system. The results obtained demonstrate that diamond supported catalyst nanomaterials are promising for methanol fuel cells.

Catalysts as Sensors—A Promising Novel Approach in Automotive Exhaust Gas Aftertreatment

Directory of Open Access Journals (Sweden)

Ralf Moos

2010-07-01

Full Text Available Sensors that detect directly and in situ the status of automotive exhaust gas catalysts by monitoring the electrical properties of the catalyst coating itself are overviewed. Examples included in this review are the in-situ determination of the electrical impedance of three-way catalysts based on ceria-zirconia solutions and of lean NOx traps of earth-alkaline based coatings, as well as approaches to determine the ammonia loading in Fe-SCR-zeolites with electrical ac measurements. Even more sophisticated approaches based on interactions with electromagnetic waves are also reviewed. For that purpose, metallic stick-like antennas are inserted into the exhaust pipe. The catalyst properties are measured in a contactless manner, directly indicating the catalyst status. The radio frequency probes gauge the oxygen loading degree of three-way catalysts, the NOx-loading of lean NOx traps, and the soot loading of Diesel particulate filters

Catalysts as Sensors—A Promising Novel Approach in Automotive Exhaust Gas Aftertreatment

Science.gov (United States)

Moos, Ralf

2010-01-01

Sensors that detect directly and in situ the status of automotive exhaust gas catalysts by monitoring the electrical properties of the catalyst coating itself are overviewed. Examples included in this review are the in-situ determination of the electrical impedance of three-way catalysts based on ceria-zirconia solutions and of lean NOx traps of earth-alkaline based coatings, as well as approaches to determine the ammonia loading in Fe-SCR-zeolites with electrical ac measurements. Even more sophisticated approaches based on interactions with electromagnetic waves are also reviewed. For that purpose, metallic stick-like antennas are inserted into the exhaust pipe. The catalyst properties are measured in a contactless manner, directly indicating the catalyst status. The radio frequency probes gauge the oxygen loading degree of three-way catalysts, the NOx-loading of lean NOx traps, and the soot loading of Diesel particulate filters. PMID:22163575

Catalysts as sensors--a promising novel approach in automotive exhaust gas aftertreatment.

Science.gov (United States)

Moos, Ralf

2010-01-01

Sensors that detect directly and in situ the status of automotive exhaust gas catalysts by monitoring the electrical properties of the catalyst coating itself are overviewed. Examples included in this review are the in-situ determination of the electrical impedance of three-way catalysts based on ceria-zirconia solutions and of lean NO(x) traps of earth-alkaline based coatings, as well as approaches to determine the ammonia loading in Fe-SCR-zeolites with electrical ac measurements. Even more sophisticated approaches based on interactions with electromagnetic waves are also reviewed. For that purpose, metallic stick-like antennas are inserted into the exhaust pipe. The catalyst properties are measured in a contactless manner, directly indicating the catalyst status. The radio frequency probes gauge the oxygen loading degree of three-way catalysts, the NO(x)-loading of lean NO(x) traps, and the soot loading of Diesel particulate filters.

Intermediate Ethanol Blends Catalyst Durability Program

Energy Technology Data Exchange (ETDEWEB)

West, Brian H; Sluder, Scott; Knoll, Keith; Orban, John; Feng, Jingyu

2012-02-01

In the summer of 2007, the U.S. Department of Energy (DOE) initiated a test program to evaluate the potential impacts of intermediate ethanol blends (also known as mid-level blends) on legacy vehicles and other engines. The purpose of the test program was to develop information important to assessing the viability of using intermediate blends as a contributor to meeting national goals for the use of renewable fuels. Through a wide range of experimental activities, DOE is evaluating the effects of E15 and E20 - gasoline blended with 15% and 20% ethanol - on tailpipe and evaporative emissions, catalyst and engine durability, vehicle driveability, engine operability, and vehicle and engine materials. This report provides the results of the catalyst durability study, a substantial part of the overall test program. Results from additional projects will be reported separately. The principal purpose of the catalyst durability study was to investigate the effects of adding up to 20% ethanol to gasoline on the durability of catalysts and other aspects of the emissions control systems of vehicles. Section 1 provides further information about the purpose and context of the study. Section 2 describes the experimental approach for the test program, including vehicle selection, aging and emissions test cycle, fuel selection, and data handling and analysis. Section 3 summarizes the effects of the ethanol blends on emissions and fuel economy of the test vehicles. Section 4 summarizes notable unscheduled maintenance and testing issues experienced during the program. The appendixes provide additional detail about the statistical models used in the analysis, detailed statistical analyses, and detailed vehicle specifications.

A detailed kinetic study of the direct ring opening of cyclohexane and methylcyclohexane over monofunctional Ir/Al{sub 2}O{sub 3} catalysts

Energy Technology Data Exchange (ETDEWEB)

Shi, Hui; Gutierrez, O.Y.; Lercher, J.A. [Technische Univ. Muenchen (Germany). Catalysis Research Center

2011-07-01

The present study analyses a series of Al{sub 2}O{sub 3}-supported iridium catalysts with different pretreatments and addresses the kinetic features and structural requirements of direct ring opening of cyclohexane and methylcyclohexane catalyzed by Ir in absence of acid-catalyzed ring contraction. Mild reaction conditions and high H{sub 2}/hydrocarbon ratios (200-1000) were used to improve accuracy of kinetic measurements and to negate deactivation. Isomerization and dehydrogenation pathways were suppressed to low extents (1-5%) over the weakly acidic catalysts under the reaction conditions applied. Three main observations are shown: 1) initial selectivity to ring opening products (ROPs) increases with iridium dispersion; 2) optimal H{sub 2} pressures differ not only between primary and secondary products, but also among ROPs and fragments; 3) the air-calcination step before catalyst reduction imposes a significant impact on both activity and product distribution. (orig.)

Experimental research of technology activating catalysts for SCR DeNOx in boiler

Science.gov (United States)

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

2018-01-01

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

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

The influence of a new fabrication procedure on the catalytic activity of ruthenium-selenium catalysts

International Nuclear Information System (INIS)

Cheng, H.; Yuan, W.; Scott, K.

2006-01-01

A new procedure has been introduced to enhance catalytic activity of ruthenium-selenium electro-catalysts for oxygen reduction, in which materials are treated under hydrogen atmosphere at elevated temperatures. The characterisation using scanning electron microscopy, energy dispersive spectroscopy or energy dispersive X-ray spectroscopy exhibited that the treatment at 400 deg. C made catalysts denser while their porous nature remained, led to a good degree of crystallinity and an optimum Se:Ru ratio. The half cell test confirms feasibility of the new procedure; the catalyst treated at 400 deg. C gave the highest reduction current (55.9 mA cm -2 at -0.4 V) and a low methanol oxidation effect coefficient (3.8%). The direct methanol fuel cell with the RuSe 400 deg. C cathode catalyst (2 mg RuSe cm -2 ) generated a power density of 33.8 mW cm -2 using 2 M methanol and 2 bar oxygen at 90 deg. C. The new procedure produced the catalysts with low decay rates. The best sample was compared to the Pt and to the reported ruthenium-selenium catalyst. Possible reasons for the observations are discussed

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.

Experimental comparison of biomass chars with other catalysts for tar reduction

NARCIS (Netherlands)

Abu El-Rub, Ziad; Bramer, Eduard A.; Brem, Gerrit

2008-01-01

In this paper the potential of using biomass char as a catalyst for tar reduction is discussed. Biomass char is compared with other known catalysts used for tar conversion. Model tar compounds, phenol and naphthalene, were used to test char and other catalysts. Tests were carried out in a fixed bed

Finding Furfural Hydrogenation Catalysts via Predictive Modelling.

Science.gov (United States)

Strassberger, Zea; Mooijman, Maurice; Ruijter, Eelco; Alberts, Albert H; Maldonado, Ana G; Orru, Romano V A; Rothenberg, Gadi

2010-09-10

We combine multicomponent reactions, catalytic performance studies and predictive modelling to find transfer hydrogenation catalysts. An initial set of 18 ruthenium-carbene complexes were synthesized and screened in the transfer hydrogenation of furfural to furfurol with isopropyl alcohol complexes gave varied yields, from 62% up to >99.9%, with no obvious structure/activity correlations. Control experiments proved that the carbene ligand remains coordinated to the ruthenium centre throughout the reaction. Deuterium-labelling studies showed a secondary isotope effect (k(H):k(D)=1.5). Further mechanistic studies showed that this transfer hydrogenation follows the so-called monohydride pathway. Using these data, we built a predictive model for 13 of the catalysts, based on 2D and 3D molecular descriptors. We tested and validated the model using the remaining five catalysts (cross-validation, R(2)=0.913). Then, with this model, the conversion and selectivity were predicted for four completely new ruthenium-carbene complexes. These four catalysts were then synthesized and tested. The results were within 3% of the model's predictions, demonstrating the validity and value of predictive modelling in catalyst optimization.

Preparation of hydrophobic Pt-catalysts for decontamination of nuclear effluents

International Nuclear Information System (INIS)

Ionita, Gh.; Popescu, I.; Retegan, T.; Stefanescu, I.

2005-01-01

Based on the long experience of the authors, in the preparation, testing and evaluation of the performances of hydrophobic catalysts, and based on the reviewed references, this paper presents up-to-date R and D activities on the preparation methods and applications of the hydrophobic catalysts, in deuterium and tritium separation. The objectives of the paper are: (1) to provide a database for selection of the most appropriate catalyst and catalytic packing for above mentioned processes, (2) to evaluate the potentiality of hydrophobic Pt-catalysts in the deuterium and tritium separation (3) to asses and to find a new procedure for preparation a new improved hydrophobic catalyst. The merits of the hydrophobic catalysts are shown in comparison to hydrophilic catalysts. As results of the review some general conclusions about the applications of hydrophobic catalysts in environmental field are as follow: (1) the hydrophobic Pt-catalysts packed in the trickle bed reactors showed a high catalytic activity and long stability; (2) the utilization of the hydrophobic Pt-catalysts for tritium removal from liquid and gaseous effluent in nuclear field was entirely confirmed on industrial scale; (3) the extension of the utilization of the hydrophobic Pt-catalysts in other new processes, which take place in presence of liquid water or high humidity are subjected to testing. (author)

Preparation of hydrophobic Pt-catalysts for decontamination of nuclear effluents

International Nuclear Information System (INIS)

Ionita, Gh.; Popescu, I.; Retegan, T.; Stefanescu, I.

2004-01-01

Based on the long experience of the authors, in the preparation, testing and evaluation of the performances of hydrophobic catalysts, and based on the reviewed references, this paper presents up-to-date R and D activities on the preparation methods and applications of the hydrophobic catalysts, in deuterium and tritium separation. The objectives of the paper are: - to provide a database for selection of the most appropriate catalyst and catalytic packing for above mentioned processes; - to evaluate the potentiality of hydrophobic Pt-catalysts in the deuterium and tritium separation; - to assess and to find a new procedure for preparation a new improved hydrophobic catalyst. The merits of the hydrophobic catalysts are shown in comparison to hydrophilic catalysts. As results of the review some general conclusions about the applications of hydrophobic catalysts in environmental field are as follows: - the hydrophobic Pt-catalysts packed in the trickle bed reactors showed a high catalytic activity and long stability; - the utilization of the hydrophobic Pt-catalysts for tritium removal from liquid and gaseous effluent in nuclear field was entirely confirmed on industrial scale; - the extension of the utilization of the hydrophobic Pt-catalysts in other new processes, which take place in presence of liquid water or high humidity are subject to testing. (authors)

Effect of Catalyst Pellet-Diameter and Basicity on Transesterification of Soybean Oil into Biodiesel using K2O/CaO-ZnO Catalyst over Hybrid Catalytic-Plasma Reactor

Directory of Open Access Journals (Sweden)

Istadi I.

2018-01-01

Full Text Available This research is aimed to study the effect of catalyst pellet-diameter and catalyst basicity on the transesterification process of soybean oil into biodiesel over a hybrid catalytic-plasma reactor. Various catalyst diameters (3, 5, and 7 mm were tested in this reaction system. Catalyst basicity was also examined by comparing fresh and used catalyst as well as with and without K2O promoter. All catalysts testing were performed in a hybrid plasma-catalytic reactor (dielectric barrier discharge – DBD type. From the results, the synergistic effects roles of the catalyst and the plasma in the transesterification process are important, in which the energetic electrons within plasma assist the reaction on the catalyst surface by an exciting bonded electron. The catalyst basicity was influenced by the composition of CaO on the catalyst as well as roles of the alkaline K2O promoter. Catalyst basicity is important in producing biodiesel with high performance. Yield of fatty acid alkyl ester (FAAE or biodiesel is slightly influenced by the catalyst diameter within the range of diameter studied.

Hydrogenation of citral into its derivatives using heterogeneous catalyst

Science.gov (United States)

Sudiyarmanto, Hidayati, Luthfiana Nurul; Kristiani, Anis; Aulia, Fauzan

2017-11-01

Citral as known as a monoterpene can be found in plants and citrus fruits. The hydrogenation of citral into its derivatives become interesting area for scientist. This compound and its derivatives can be used for many application in pharmaceuticals and food areas. The development of heterogeneous catalysts become an important aspect in catalytic hydrogenation citral process. Nickel supported catalysts are well known as hydrogenation catalyst. These heterogeneous catalysts were tested their catalytic activity in hydrogenation of citral. The effect of various operation conditions, in term of feed concentration, catalyst loading, temperature, and reaction time were also studied. The liquid products produced were analyzed by using Gas Chromatography-Mass Spectroscopy (GC-MS). The result of catalytic activity tests showed nickel skeletal catalyst exhibits best catalytic activity in hydrogenation of citral. The optimum of operation condition was achieved in citral concentration 0.1 M with nickel skeletal catalyst loading of 10% (w/w) at 80 °C and 20 bar for 2 hours produced the highest conversion as of 64.20% and the dominant product resulted was citronellal as of 56.48%.

The Effect of Time dealumination and Solvent Concentration in Synthesis of Zeolite Catalyst and Catalytic Test for DiEthyl Ether Production Process

International Nuclear Information System (INIS)

Widayat; Roesyadi, A.; Rachimoellah, M.

2009-01-01

Ethanol is an alternative energy, but its has three distinct disadvantages as a transportation fuel. Its availability is currently limited, and it has a lower volumetric heating value and a lower Reid vapour pressure (RVP) than gasoline. This paper focuses for this disadvantages and to solve this problem can do with converts ethanol to DiEthyl Ether product. This research produced DiEthyl Ether by ethanol dehydration process with zeolite as catalyst. The catalyst synthesis from natural material from District Gunung Kidul, Indonesia. The catalyst produced with dealumination, neutralization, drying and calcination processes. The zeolite catalyst was analysed of Si/Al, X-ray Diffraction and specific surface area. The catalyst product then used for ethanol dehydration to produce DiEthyl Ether. The results shown the biggest surface area is 184,52 m 2 /gram at catalyst production at 10 hours for time dealumination. The crystallite of catalyst product is similar like shown at diffractogram of XRD analysis. The ratio Si/Al biggest is 313.7 that obtaining at catalyst production with 7 hours for time dealumination. The catalytic test use fixed bed reactor with 1 inci diameter and ethanol fermentation both as feed. The operation condition is 150 deg. C at temperature and atmosphere pressure. The compounds product in liquid phase are diethyl ether, methanol and water.

Characteristics improvement of hydrophobic polytetrafluoroethylene-platinum catalysts for tritium separation

International Nuclear Information System (INIS)

Popescu, I.; Ionita, Gh.; Dobrinescu, D.; Varlam, C.; Stefanescu, I.

2006-01-01

Full text: Based on the long experience of the authors in the preparation, testing and evaluation of the performances of hydrophobic catalysts and based on the reviewed references, this paper presents up-to-date R and D activities on the preparation methods and applications of the hydrophobic catalysts in tritium separation. The objectives of the paper are: how to improve the characteristics and performance of platinum hydrophobic catalysts; to assess and find a new procedure for the preparation of a new improved hydrophobic catalyst. From reviewed references one can conclude that platinum is the most active and efficient catalytic metal while the polytetrafluoroethylene is the best wet-proofing agent. A new improved hydrophobic Pt-catalyst has been proposed and its testing is now underway. The main steps and experimental conditions of preparation are thoroughly discussed. A new wet-proofing agent and new binders (titanium dioxide, cerium dioxide, zirconium dioxide) with a catalytic role are proposed and tested. The physico-structural parameters of the improved catalyst have been determined and are discussed in detail. The new proposal is a promising idea to improve the performance of conventional hydrophobic Pt-catalysts. (authors)

Structure-activity relationship of surfactant for preparing DMFC anodic catalyst

International Nuclear Information System (INIS)

Su Yi; Xue Xinzhong; Xu Weilin; Liu Changpeng; Xing Wei; Zhou Xiaochun; Tian Tian; Lu Tianhong

2006-01-01

Three kinds of surfactants as stabilizer were applied to the preparation of electrocatalysts for direct methanol fuel cell (DMFC). The catalysts have been characterized by examining their catalytic activities, morphologies and particle sizes by means of cyclic voltammetry, chronoamperometry, X-ray diffraction and transmission electron microscopy (TEM). It is found that the surfactants with different structures have a significantly influence on the catalyst shape and activity. The catalysts prepared with non-ionic surfactants as the stabilizer show higher activity for direct oxidation of methanol. The structure-activity relationship (SAR) analysis has been explored and the effect of hydrophile-lipophile balance (HLB value) has also been discussed

Ir catalysts: Preventing CH3COOH formation in ethanol oxidation

Science.gov (United States)

Miao, Bei; Wu, Zhipeng; Xu, Han; Zhang, Minhua; Chen, Yifei; Wang, Lichang

2017-11-01

Current catalysts used for ethanol oxidation reaction (EOR) cannot effectively prevent CH3COOH formation, and thus become a major hindrance for direct ethanol fuel cell applications. We report an Ir catalyst that shows great promise for a complete EOR based on density functional theory calculations using PBE functional. The reaction barrier on Ir(1 0 0) was found to be 2.10 eV for CH3COOH formation, which is much higher than currently used Pd and Pt, and 0.57 eV for Csbnd C bond cleavage in CHCO species, which are comparable to Pd and Pt. The result suggests future directions for studying optimal complete EOR catalysts.

ADVANCED BYPRODUCT RECOVERY: DIRECT CATALYTIC REDUCTION OF SO2 TO ELEMENTAL SULFUR; FINAL

International Nuclear Information System (INIS)

Robert S. Weber

1999-01-01

Arthur D. Little, Inc., together with its commercialization partner, Engelhard Corporation, and its university partner Tufts, investigated a single-step process for direct, catalytic reduction of sulfur dioxide from regenerable flue gas desulfurization processes to the more valuable elemental sulfur by-product. This development built on recently demonstrated SO(sub 2)-reduction catalyst performance at Tufts University on a DOE-sponsored program and is, in principle, applicable to processing of regenerator off-gases from all regenerable SO(sub 2)-control processes. In this program, laboratory-scale catalyst optimization work at Tufts was combined with supported catalyst formulation work at Engelhard, bench-scale supported catalyst testing at Arthur D. Little and market assessments, also by Arthur D. Little. Objectives included identification and performance evaluation of a catalyst which is robust and flexible with regard to choice of reducing gas. The catalyst formulation was improved significantly over the course of this work owing to the identification of a number of underlying phenomena that tended to reduce catalyst selectivity. The most promising catalysts discovered in the bench-scale tests at Tufts were transformed into monolith-supported catalysts at Engelhard. These catalyst samples were tested at larger scale at Arthur D. Little, where the laboratory-scale results were confirmed, namely that the catalysts do effectively reduce sulfur dioxide to elemental sulfur when operated under appropriate levels of conversion and in conditions that do not contain too much water or hydrogen. Ways to overcome those limitations were suggested by the laboratory results. Nonetheless, at the end of Phase I, the catalysts did not exhibit the very stringent levels of activity or selectivity that would have permitted ready scale-up to pilot or commercial operation. Therefore, we chose not to pursue Phase II of this work which would have included further bench-scale testing

Synthesis and characterization of MCM-41-supported nano zirconia catalysts

Directory of Open Access Journals (Sweden)

Mohamed S. Abdel Salam

2015-03-01

Full Text Available Series of MCM-41 supported sulfated Zirconia (SZ catalysts with different loadings (2.5–7.5% wt. were prepared using direct impregnation method. The acquired solid catalysts were characterized structurally and chemically using X-RD, HRTEM, BET, FT-IR, Raman spectroscopy and TPD analysis. The acidity of the solid catalysts was investigated through cumene cracking and isopropanol dehydration at different temperatures. As the SZ loading increases, the surface acidity of the mesoporous catalysts was enhanced, this was reflected by the higher catalytic activity toward cumene cracking and isopropanol dehydration.

Pd/NbOPO₄ multifunctional catalyst for the direct production of liquid alkanes from aldol adducts of furans.

Science.gov (United States)

Xia, Qi-Neng; Cuan, Qian; Liu, Xiao-Hui; Gong, Xue-Qing; Lu, Guan-Zhong; Wang, Yan-Qin

2014-09-08

Great efforts have been made to convert renewable biomass into transportation fuels. Herein, we report the novel properties of NbO(x)-based catalysts in the hydrodeoxygenation of furan-derived adducts to liquid alkanes. Excellent activity and stability were observed with almost no decrease in octane yield (>90% throughout) in a 256 h time-on-stream test. Experimental and theoretical studies showed that NbO(x) species play the key role in C-O bond cleavage. As a multifunctional catalyst, Pd/NbOPO4 plays three roles in the conversion of aldol adducts into alkanes: 1) The noble metal (in this case Pd) is the active center for hydrogenation; 2) NbO(x) species help to cleave the C-O bond, especially of the tetrahydrofuran ring; and 3) a niobium-based solid acid catalyzes the dehydration, thus enabling the quantitative conversion of furan-derived adducts into alkanes under mild conditions. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A Facile Synthesis of Hollow Palladium/Copper Alloy Nanocubes Supported on N-Doped Graphene for Ethanol Electrooxidation Catalyst

Directory of Open Access Journals (Sweden)

Zhengyu Bai

2015-04-01

Full Text Available In this paper, a catalyst of hollow PdCu alloy nanocubes supported on nitrogen-doped graphene support (H-PdCu/ppy-NG is successfully synthesized using a simple one-pot template-free method. Two other catalyst materials such as solid PdCu alloy particles supported on this same nitrogen-doped graphene support (PdCu/ppy-NG and hollow PdCu alloy nanocubes supported on the reduced graphene oxide support (H-PdCu/RGO are also prepared using the similar synthesis conditions for comparison. It is found that, among these three catalyst materials, H-PdCu/ppy-NG gives the highest electrochemical active area and both the most uniformity and dispersibility of H-PdCu particles. Electrochemical tests show that the H-PdCu/ppy-NG catalyst can give the best electrocatalytic activity and stability towards the ethanol electrooxidation when compared to other two catalysts. Therefore, H-PdCu/ppy-NG should be a promising catalyst candidate for anodic ethanol oxidation in direct ethanol fuel cells.

Structure and catalytic activity of regenerated spent hydrotreating catalysts

Energy Technology Data Exchange (ETDEWEB)

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

1992-11-01

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

Finding Furfural Hydrogenation Catalysts via Predictive Modelling

Science.gov (United States)

Strassberger, Zea; Mooijman, Maurice; Ruijter, Eelco; Alberts, Albert H; Maldonado, Ana G; Orru, Romano V A; Rothenberg, Gadi

2010-01-01

Abstract We combine multicomponent reactions, catalytic performance studies and predictive modelling to find transfer hydrogenation catalysts. An initial set of 18 ruthenium-carbene complexes were synthesized and screened in the transfer hydrogenation of furfural to furfurol with isopropyl alcohol complexes gave varied yields, from 62% up to >99.9%, with no obvious structure/activity correlations. Control experiments proved that the carbene ligand remains coordinated to the ruthenium centre throughout the reaction. Deuterium-labelling studies showed a secondary isotope effect (kH:kD=1.5). Further mechanistic studies showed that this transfer hydrogenation follows the so-called monohydride pathway. Using these data, we built a predictive model for 13 of the catalysts, based on 2D and 3D molecular descriptors. We tested and validated the model using the remaining five catalysts (cross-validation, R2=0.913). Then, with this model, the conversion and selectivity were predicted for four completely new ruthenium-carbene complexes. These four catalysts were then synthesized and tested. The results were within 3% of the model’s predictions, demonstrating the validity and value of predictive modelling in catalyst optimization. PMID:23193388

The role of zeolites in the deactivation of multifunctional fischer-tropsch synthesis catalysts: the interaction between HZSM-5 and Fe-based Ft-catalysts

Directory of Open Access Journals (Sweden)

P. C. Zonetti

2013-12-01

Full Text Available In order to produce gasoline directly from syngas, HZSM-5 can be added to the Fischer-Tropsch catalyst. However, this catalytic system shows an important deactivation rate. Aiming at describing this phenomenon, Fe-based catalysts and physical mixtures containing these catalysts and HZSM-5 were employed in this reaction. All these systems were characterized using the following techniques: XRD, XPS, TPR and TPD of CO. This work shows that HZSM-5 interacts with the Fe-based Fischer-Tropsch catalyst during the reduction step, decreasing the Fe concentration on the catalytic surface and thus lowering the activity of the catalytic system in the Fischer-Tropsch Synthesis.

The role of zeolites in the deactivation of multifunctional Fischer-Tropsch Synthesis catalysts: the interaction between HZSM-5 and Fe-based FT-catalysts

International Nuclear Information System (INIS)

Zonetti, P.C.; Gaspar, A.B.; Mendes, F.M.T.; Appel, L.G.; Avillez, R. R. de; Sousa-Aguiar, E.F.

2013-01-01

In order to produce gasoline directly from syngas, HZSM-5 can be added to the Fischer-Tropsch catalyst. However, this catalytic system shows an important deactivation rate. Aiming at describing this phenomenon, Fe-based catalysts and physical mixtures containing these catalysts and HZSM-5 were employed in this reaction. All these systems were characterized using the following techniques: XRD, XPS, TPR and TPD of CO. This work shows that HZSM-5 interacts with the Fe-based Fischer-Tropsch catalyst during the reduction step, decreasing the Fe concentration on the catalytic surface and thus lowering the activity of the catalytic system in the Fischer-Tropsch Synthesis. (author)

The role of zeolites in the deactivation of multifunctional Fischer-Tropsch Synthesis catalysts: the interaction between HZSM-5 and Fe-based FT-catalysts

Energy Technology Data Exchange (ETDEWEB)

Zonetti, P.C.; Gaspar, A.B.; Mendes, F.M.T.; Appel, L.G., E-mail: lucia.appel@int.gov.br [Instituto Nacional de Tecnologia (INT/MCT), Rio de Janeiro, RJ (Brazil); Avillez, R. R. de [Pontificia Universidade Catolica do Rio de Janeiro (PUC-Rio), RJ (Brazil); Sousa-Aguiar, E.F. [Centro de Pesquisa Leopoldo Americo Miguez de Mello (CENPES/PETROBRAS), Rio de Janeiro, RJ (Brazil)

2013-10-15

In order to produce gasoline directly from syngas, HZSM-5 can be added to the Fischer-Tropsch catalyst. However, this catalytic system shows an important deactivation rate. Aiming at describing this phenomenon, Fe-based catalysts and physical mixtures containing these catalysts and HZSM-5 were employed in this reaction. All these systems were characterized using the following techniques: XRD, XPS, TPR and TPD of CO. This work shows that HZSM-5 interacts with the Fe-based Fischer-Tropsch catalyst during the reduction step, decreasing the Fe concentration on the catalytic surface and thus lowering the activity of the catalytic system in the Fischer-Tropsch Synthesis. (author)

Atomic Layer Deposited Catalysts for Fuel Cell Applications

DEFF Research Database (Denmark)

Johansson, Anne-Charlotte Elisabeth Birgitta

catalyst toward the methanol oxidation reaction (MOR). In the work described in this PhD dissertation, two series of Pt-Ru ALD catalysts supported on nitrogen-doped multi-walled carbon nanotubes (N-CNTs) have been evaluated toward the CO oxidation and MOR at room temperature in a three......The micro direct methanol fuel cell (µDMFC) has been proposed as a candidate to power portable applications. The device can operate at room temperature on inexpensive, energy-dense methanol fuel, and it can be easily "recharged" by fuel refilling. Microfabrication techniques could be one route......-electrode electrochemical cell. The first series was comprised of Pt-Ru ALD catalysts of various Ru compositions, between 0 and 100 at.%. For the compositions investigated, the best catalyst had a Ru composition of 29 at.%. In the second series Ru-decorated Pt catalysts of various Ru loadings, i.e., various Ru ALD cycles...

On the potential of nickel catalysts for steam reforming in membrane reactors

Energy Technology Data Exchange (ETDEWEB)

Pieterse, J.A.Z.; Boon, J.; Van Delft, Y.C.; Dijkstra, J.W.; Van den Brink, R.W. [Energy research Center of the Netherlands, P.O. Box 1, 1755 ZG Petten (Netherlands)

2010-10-15

Hydrogen membrane reactors have been identified as a promising option for hydrogen production for power generation from natural gas with pre-combustion decarbonisation. While Pd or Pd-alloy membranes already provide good hydrogen permeances the most suitable catalyst design for steam reforming in membrane reactors (SRMR) is yet to be identified. This contribution aims to provide insight in the suitability of nickel based catalysts in SRMR. The use of nickel (Ni) catalysts would benefit the cost-effectiveness of membrane reactors and therefore its feasibility. For this, the activity of nickel catalysts in SRMR was assessed with kinetics reported in literature. A 1D model was composed in order to compare the hydrogen production rates derived from the kinetics with the rate of hydrogen withdrawal by permeation. Catalyst stability was studied by exposing the catalysts to reformate gas with two different H/C ratios to mimic the hydrogen lean reformate gas in the membrane reactor. For both the activity (modeling) and stability study the Ni-based catalysts were compared to relevant catalyst compositions based on rhodium (Rh). Using the high pressure kinetics reported for Al2O3 supported Rh and MgAl2O4 and Al2O3 supported Ni catalyst it showed that Ni and Rh catalysts may very well provide similar hydrogen production rates. Interestingly, the stability of Ni-based catalysts proved to be superior to precious metal based catalysts under exposure to simulated reformate feed gas with low H/C molar ratio. A commercial (pre-)reforming Ni-based catalyst was selected for further testing in an experimental membrane reactor for steam reforming at high pressure. During the test period 98% conversion at 873 K could be achieved. The conversion was adjusted to approximately 90% and stable conversion was obtained during the test period of another 3 weeks. Nonetheless, carbon quantification tests of the Ni catalyst indicated that a small amount of carbon had deposited onto the catalyst

Evaluation of AECL catalysts for hydrogen fuel-cell applications. Paper no. IGEC-1-073

International Nuclear Information System (INIS)

Li, J.; Suppiah, S.; Li, H.; Kutchcoskie, K.J.; Strikwerda, S.

2005-01-01

AECL has been engaged in the promotion of the nuclear-hydrogen economy, which envisions that hydrogen fuel cells will generate power using hydrogen as fuel produced by nuclear energy. Since AECL's catalysts developed for the production, upgrading and detritiation of heavy water are very similar to commercial fuel-cell catalysts, a program was initiated to evaluate AECL catalysts for fuel-cell applications. As a first step in this effort, a half-cell test facility was set up to characterize the performance of catalysts for hydrogen fuel cells. This paper outlines the results obtained from cathodic reduction of oxygen in a 0.5 M sulphuric acid solution on a rotating disc electrode at 65 o C. The performance of the catalysts was characterized using standard electrochemical methods including cyclic voltammetry, Voltammogram/Tafel plots and short-term stability plots. Several monometallic Pt and Pt-based bimetallic catalysts were tested and compared with a commercially available catalyst for fuel-cell applications. AECL's monometallic Pt catalysts showed comparable or better activities than commercial catalysts with similar Pt loading. An AECL Pt-based bimetallic catalyst has shown superior performance to a monometallic Pt catalyst with similar Pt loading. Evaluation of various catalyst formulations is ongoing on the half-cell facility at AECL. Further investigation of promising catalysts identified from half-cell test is also being carried out in single fuel cell on test stations under normal fuel-cell operating conditions. (author)

Final Report: Cathode Catalysis in Hydrogen/Oxygen Fuel Cells: New Catalysts, Mechanism, and Characterization

Energy Technology Data Exchange (ETDEWEB)

Gewirth, Andrew A. [Univ. of Illinois, Urbana, IL (United States). Dept. of Chemistry; Kenis, Paul J. [Univ. of Illinois, Urbana, IL (United States). Dept. of Chemical and Biomolecular Engineering; Nuzzo, Ralph G. [Univ. of Illinois, Urbana, IL (United States). Dept. of Chemistry; Rauchfuss, Thomas B. [Univ. of Illinois, Urbana, IL (United States). Dept. of Chemistry

2016-01-18

In this research, we prosecuted a comprehensive plan of research directed at developing new catalysts and new understandings relevant to the operation of low temperature hydrogen-oxygen fuel cells. The focal point of this work was one centered on the Oxygen Reduction Reaction (ORR), the electrochemical process that most fundamentally limits the technological utility of these environmentally benign energy conversion devices. Over the period of grant support, we developed new ORR catalysts, based on Cu dimers and multimers. In this area, we developed substantial new insight into design rules required to establish better ORR materials, inspired by the three-Cu active site in laccase which has the highest ORR onset potential of any material known. We also developed new methods of characterization for the ORR on conventional (metal-based) catalysts. Finally, we developed a new platform to study the rate of proton transfer relevant to proton coupled electron transfer (PCET) reactions, of which the ORR is an exemplar. Other aspects of work involved theory and prototype catalyst testing.

Facile synthesis of a platinum-lead oxide nanocomposite catalyst with high activity and durability for ethanol electrooxidation.

Science.gov (United States)

Yang, Wei-Hua; Wang, Hong-Hui; Chen, De-Hao; Zhou, Zhi-You; Sun, Shi-Gang

2012-12-21

Aimed at searching for highly active and stable nano-scale Pt-based catalysts that can improve significantly the energy conversion efficiency of direct ethanol fuel cells (DEFCs), a novel Pt-PbO(x) nanocomposite (Pt-PbO(x) NC) catalyst with a mean size of 3.23 nm was synthesized through a simple wet chemistry method without using a surfactant, organometallic precursors and high temperature. Electrocatalytic tests demonstrated that the as-prepared Pt-PbO(x) NC catalyst possesses a much higher catalytic activity and a longer durability than Pt nanoparticles (nm-Pt) and commercial Pt black catalysts for ethanol electrooxidation. For instance, Pt-PbO(x) NC showed an onset potential that was 30 mV and 44 mV less positive, together with a peak current density 1.7 and 2.6 times higher than those observed for nm-Pt and Pt black catalysts in the cyclic voltammogram tests. The ratio of current densities per unit Pt mass on Pt-PbO(x) NC, nm-Pt and Pt black catalysts is 27.3 : 3.4 : 1 for the long-term (2 hours) chronoamperometric experiments measured at -0.4 V (vs. SCE). In situ FTIR spectroscopic studies revealed that the activity of breaking C-C bonds of ethanol of the Pt-PbO(x) NC is as high as 5.17 times that of the nm-Pt, which illustrates a high efficiency of ethanol oxidation to CO(2) on the as-prepared Pt-PbO(x) NC catalyst.

Effect of catalyst on melamine-formaldehyde organic aerogel

International Nuclear Information System (INIS)

Sun Zhipeng; Yang Xi; Fu Zhibing; Zhong Minglong; Wang Chaoyang; Ma Kangfu; Huang Xiaoli; Chang Lijuan

2013-01-01

A series of melamine-formaldehyde(MF) organic aerogel templates were prepared with different categories and concentration of catalyst. Their molecular structure, thermal stability and pore structure were tested by Fourier transform infrared spectroscopy, thermogravimetric analysis and nitrogen adsorption. It is indicated that the type and concentration of catalyst do not affect molecular structure and thermal stability of the MF organic aerogel template. The specific surface area and pore volume of the MF organic aerogel template using Na 2 CO 3 as catalyst are higher than those using NaOH, NaHCO 3 as catalyst. When the ratio of the concentration of melamine to that of catalyst is 500, the specific surface area is maximized. (authors)

Hydrophobic catalyst mixture for the isotopic exchange reaction between hydrogen and water

Energy Technology Data Exchange (ETDEWEB)

Paek, S.; Ahn, D. H.; Choi, H. J.; Kim, K. R.; Lee, M.; Yim, S. P.; Chung, H. [KAERI, Taejon (Korea, Republic of)

2005-11-15

Pt/SDBC catalyst, which is used for the hydrogen-water isotopic exchange reaction, was prepared. The various properties of the catalyst, such as the thermal stability, pore structure and the platinum dispersion, were investigated. A hydrophobic Pt/SDBC catalyst which has been developed for the LPCE column of the WTRF (Wolsong Tritium Removal Facility) was tested in a trickle bed reactor. An experimental apparatus was built for the test of the catalyst at various temperatures and gas velocities.

Hydrophobic catalyst mixture for the isotopic exchange reaction between hydrogen and water

International Nuclear Information System (INIS)

Paek, S.; Ahn, D. H.; Choi, H. J.; Kim, K. R.; Lee, M.; Yim, S. P.; Chung, H.

2005-01-01

Pt/SDBC catalyst, which is used for the hydrogen-water isotopic exchange reaction, was prepared. The various properties of the catalyst, such as the thermal stability, pore structure and the platinum dispersion, were investigated. A hydrophobic Pt/SDBC catalyst which has been developed for the LPCE column of the WTRF (Wolsong Tritium Removal Facility) was tested in a trickle bed reactor. An experimental apparatus was built for the test of the catalyst at various temperatures and gas velocities

Study of Pd-Au/MWCNTs formic acid electrooxidation catalysts

Energy Technology Data Exchange (ETDEWEB)

Mikolajczuk, Anna; Borodzinski, Andrzej; Kedzierzawski, Piotr; Lesiak, Beata [Institute of Physical Chemistry, Polish Academy of Sciences, ul. Kasprzaka 44/52, 01-224 Warszawa (Poland); Stobinski, Leszek [Institute of Physical Chemistry, Polish Academy of Sciences, ul. Kasprzaka 44/52, 01-224 Warszawa (Poland); Faculty of Materials Science and Engineering, Warsaw University of Technology, ul. Woloska 141, 02-507 Warsaw (Poland); Koever, Laszlo; Toth, Jozsef [Institute of Nuclear Research, Hungarian Academy of Sciences (ATOMKI), P. O. Box 51, 4001 Debrecen (Hungary); Lin, Hong-Ming [Department of Materials Engineering, Tatung University, 40, Chungshan N. Rd., 3rd Sec, 104, Taipei (China)

2010-12-15

The Pd-Au multiwall carbon nanotubes (MWCNTs) supported catalyst exhibits higher power density in direct formic acid fuel cell (DFAFC) than similar Pd/MWCNTs catalyst. The Pd-Au/MWCNTs catalyst also exhibits higher activity and is more stable in electrooxidation reaction of formic acid during cyclic voltammetry (CV) measurements. After preparation by polyol method, the catalyst was subjected to two type of treatments: (I) annealing at 250 C in 100% of Ar, (II) reducing in 5% of H{sub 2} in Ar atmosphere at 200 C. It was observed that the catalyst after treatment I was completely inactive, whereas after treatment II exhibited high activity. In order to explain this effect the catalysts were characterized by electron spectroscopy methods. The higher initial catalytic activity of Pd-Au/MWCNTs catalyst than Pd/MWCNTs catalyst in reaction of formic acid electrooxidation was attributed to electronic effect of gold in Pd-Au solution, and larger content of small Au nanoparticles of 1 nm size. The catalytic inactivity of Pd-Au/MWCNTs catalysts annealed in argon is attributed to carbon amorphous overlayer covering of Pd oxide shell on the metallic nanoparticles. (Copyright copyright 2010 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Effect of the solvent in the catalyst ink preparation on the properties and performance of unsupported PtRu catalyst layers in direct methanol fuel cells

International Nuclear Information System (INIS)

Alcaide, Francisco; Álvarez, Garbiñe; Cabot, Pere L.; Genova-Koleva, Radostina; Grande, Hans-Jürgen; Miguel, Oscar

2017-01-01

The effect of the organic solvent polarity on the properties of unsupported PtRu catalyst inks and on the performance of the catalyst layers prepared with them for the methanol electrooxidation, has been studied. The light scattering results indicate that the PtRu-Nafion ® aggregates in the inks prepared with n-butyl acetate (NBA) are larger than those prepared with 2-propanol (IPA). The lower polarity of the former favours the aggregation of Nafion ® and nanoparticles. The electron microscopy images and porosimetry measurements of the catalyst layers show that the secondary pore volume between the agglomerates is larger for NBA. The linear sweep voltammetry and eis results for the methanol electrooxidation in the three-electrode cell denote the higher active surface area for NBA and comparable specific oxidation rates of the intermediates in both catalysts layers. The current densities for PtRu anode catalyst layers in single DMFC are higher when the solvent is NBA, the mass transport limitations being much more apparent with IPA. The adapted transmission line equivalent circuit to interpret the impedance results in single DMFC indicates that the proton resistance for NBA is significantly lower than for IPA, thus suggesting that the greater number of accessible active sites for methanol oxidation in the former are well connected to the Nafion ® ionomers and easier transported to the membrane.

Use of phyllosilicates in electrochemical devices: possible use of sepiolite as a support of catalysts in direct alcohol fuel cells (DAFC); Utilizacao de filosilicatos em dispositivos eletroquimicos: possivel uso da sepiolita como suporte de catalisadores em celulas a combustivel com uso direto de etanol (DAFC)

Energy Technology Data Exchange (ETDEWEB)

Parra-Silva, J.; Silva, A.C.; Mello-Castanho, S.R.H. [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil); Cerpa, A. [Universidad Europea de Madrid, Madrid (Spain)

2014-07-01

Direct alcohol Fuel cells (DAFC) are interesting to use Brazil for reasons of fuel logistics and availability. The catalysts used in these devices to promote the oxidation of alcohol at the anode need to be fixed on a substrate which must provide high specific surface area, porosity, chemical and thermal resistance, this target can be achieved with the characteristics sepiolite. This paper proposes sepiolite as catalyst support for DAFC. Sepiolite is a phyllosilicate with double layered tetrahedral silicon cells and fibrillar structure. Catalysts (Pt / Sb / Sn) were prepared by cation substitution method and tested by cyclic voltammetry. Techniques as XRD and FT-IR were also used for characterizing materials. Was obtained up to 35 mA / g (Pt) peak current (redox ethanol) indicating the possibility of sepiolite technology development to use un proposed purpose. (author)

A two-stage fixed-bed reactor for direct hydrotreatment of volatiles from the hydropyrolysis of biomass: effect of catalyst temperature, pressure and catalyst ageing time on product characteristics

Energy Technology Data Exchange (ETDEWEB)

Pindoria, R.V.; Megaritis, A.; Herod, A.A.; Kandiyoti, R. [Imperial College of Science, Technology and Medicine, London (United Kingdom). Dept. of Chemical Engineering and Chemical Technology

1998-12-01

This investigation involved the hydropyrolysis of biomass (eucalyptus globulus) and the immediate catalytic hydrocracking of pyrolytic oils in the second stage of the reactor. The effects of temperature, pressure and the catalyst ageing time on the final product tar have been studied using the catalyst Zeolite H-ZSM5. The catalytically hydrocracked tar/oil products were characterised and compared with the hydropyrolysis product from the first stage of the reactor to determine the effect of catalytic hydrocracking. The carbon deposition on the catalyst has been examined using thermogravimetric analysis. The tar yields after catalytic hydrocracking decreased with increasing pressure and temperature of the cracking stage. The tar yields at 10 bar pressure were greater than those at 40 bar pressure. The fresh zeolite catalyst trapped more than 40% of the product from the hydropyrolysis stage and TGA evidence indicated that this was not as carbon deposition but as volatiles trapped in the zeolite matrix. Reuse of the catalyst resulted in little more uptake of volatiles; however, extended use of the catalyst did not result in increased yields of liquid products but in increased production of light volatiles or gas. The H-ZSM5 catalyst appeared to act as a more active cracking catalyst rather than to promote hydrogenation or deoxygenation of the liquids produced in the hydropyrolysis stage. Characterisation of the liquids by SEC and UV fluorescence indicated that structural changes were relatively minor despite the significant changes in yields of liquids with process conditions. Available reaction routes do not appear to allow specific deoxygenation pathways to predominate without disintegration of parent molecules to lighter volatiles, under the conditions used here. 41 refs., 10 figs., 4 tabs.

Assessment of research needs for advanced heterogeneous catalysts for energy applications. Final report: Volume 2, Topic reports

Energy Technology Data Exchange (ETDEWEB)

Mills, G.A.

1994-04-01

This report assesses the direction, technical content, and priority of research needs judged to provide the best chance of yielding new and improved heterogeneous catalysts for energy-related applications over the period of 5-20 years. It addresses issues of energy conservation, alternate fuels and feedstocks, and the economics and applications that could alleviate pollution from energy processes. Recommended goals are defined in 3 research thrusts: catalytic science, environmental protection by catalysis, and industrial catalytic applications. This study was conducted by an 11-member panel of experts from industry and academia, including one each from Japan and Europe. This volume first presents an in-depth overview of the role of catalysis in future energy technology in chapter 1; then current catalytic research is critically reviewed and research recommended in 8 topic chapters: catalyst preparation (design and synthesis), catalyst characterization (structure/function), catalyst performance testing, reaction kinetics/reactor design, catalysis for industrial chemicals, catalysis for electrical applications (clean fuels, pollution remediation), catalysis for control of exhaust emissions, and catalysts for liquid transportation fuels from petroleum, coal, residual oil, and biomass.

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.

Selective production of arenes via direct lignin upgrading over a niobium-based catalyst

Science.gov (United States)

Shao, Yi; Xia, Qineng; Dong, Lin; Liu, Xiaohui; Han, Xue; Parker, Stewart F.; Cheng, Yongqiang; Daemen, Luke L.; Ramirez-Cuesta, Anibal J.; Yang, Sihai; Wang, Yanqin

2017-07-01

Lignin is the only large-volume renewable source of aromatic chemicals. Efficient depolymerization and deoxygenation of lignin while retaining the aromatic functionality are attractive but extremely challenging. Here we report the selective production of arenes via direct hydrodeoxygenation of organosolv lignin over a porous Ru/Nb2O5 catalyst that enabled the complete removal of the oxygen content from lignin. The conversion of birch lignin to monomer C7-C9 hydrocarbons is nearly quantitative based on its monomer content, with a total mass yield of 35.5 wt% and an exceptional arene selectivity of 71 wt%. Inelastic neutron scattering and DFT calculations confirm that the Nb2O5 support is catalytically unique compared with other traditional oxide supports, and the disassociation energy of Caromatic-OH bonds in phenolics is significantly reduced upon adsorption on Nb2O5, resulting in its distinct selectivity to arenes. This one-pot process provides a promising approach for improved lignin valorization with general applicability.

Empirical Evaluation of Directional-Dependence Tests

Science.gov (United States)

Thoemmes, Felix

2015-01-01

Testing of directional dependence is a method to infer causal direction that recently has attracted some attention. Previous examples by e.g. von Eye and DeShon (2012a) and extensive simulation studies by Pornprasertmanit and Little (2012) have demonstrated that under specific assumptions, directional-dependence tests can recover the true causal…

Biodiesel production from waste cooking oil using KBr impregnated CaO as catalyst

International Nuclear Information System (INIS)

Mahesh, Sneha E.; Ramanathan, Anand; Begum, K.M. Meera S.; Narayanan, Anantharaman

2015-01-01

Highlights: • KBr impregnated CaO has been used as heterogeneous catalyst. • Efficient use of waste cooking oil as feedstock. • Response Surface Methodology was used to optimize process parameters. - Abstract: This research paper deals with the synthesis of a heterogeneous catalyst (KBr/CaO) from commercial calcium oxide and potassium bromide by wet impregnation method. This solid catalyst was tested for transesterification of waste cooking oil (WCO). The synthesized catalyst was characterized by Fourier Transform Infrared spectrometry (FTIR), X-ray Diffraction (XRD) and Scanning Electron Microscopy (SEM) techniques. Transesterification reaction parameters were varied to obtain the maximum yield of biodiesel. Response Surface Methodology (RSM) using Central Composite Design (CCD) was employed to study the effect of the process variables like methanol to oil ratio, catalyst loading and reaction time. The optimum conditions obtained using regression models were found to be 12:1 methanol: oil ratio, 3 wt% catalyst loading and 1.8 h reaction time. The composition of FAME was determined using Gas Chromatography–Mass Spectrometry (GC–MS). The performance and emission characteristics for various blends of biodiesel (B10, B20, B50 and B100) were investigated in a four stroke direct injection diesel engine. The results indicated that the brake thermal efficiency, particulate matter, unburned hydrocarbons, carbon monoxide emissions reduced with increased concentration of biodiesel in the fuel blends, whereas the specific fuel consumption, NO x emissions and exhaust gas temperature increased

Catalysts, methods of making catalysts, and methods of use

KAUST Repository

Renard, Laetitia; El Eter, Mohamad; Caps, Valerie; Basset, Jean-Marie

2014-01-01

Embodiments of the present disclosure provide for catalysts, methods of making catalysts, methods of using catalysts, and the like. In an embodiment, the method of making the catalysts can be performed in a single step with a metal nanoparticle precursor and a metal oxide precursor, where a separate stabilizing agent is not needed.

Catalysts, methods of making catalysts, and methods of use

KAUST Repository

Renard, Laetitia

2014-03-06

Embodiments of the present disclosure provide for catalysts, methods of making catalysts, methods of using catalysts, and the like. In an embodiment, the method of making the catalysts can be performed in a single step with a metal nanoparticle precursor and a metal oxide precursor, where a separate stabilizing agent is not needed.

What Is Direct-to-Consumer Genetic Testing?

Science.gov (United States)

... consumer genetic testing? What kinds of direct-to-consumer genetic tests are available? What is genetic ancestry testing? What are the benefits and risks of direct-to-consumer genetic testing? ...

Test and survey on a next generation coal liquefying catalyst. Coal molecule scientific test and survey as the base for commercializing the coal liquefying technology; Jisedai sekitan ekika shokubai shiken chosa. Sekitan ekika gijutsu shogyoka kiban to shite no sekitan bunshi kagaku shiken chosa

Energy Technology Data Exchange (ETDEWEB)

NONE

1998-03-01

The test and survey on a next generation coal liquefying catalyst present a new proposal to raise catalytic activity in coal liquefaction, and perform demonstration experiments in a laboratory scale to search for possibility of developing a new coal liquefying catalyst from various viewpoints. To explain, discussions were given on the catalyst to perform the followings: liquefaction under extremely mild conditions by using ultra strong acids not limited only to metals; ion exchange method and swell carrying method to raise catalyst dispersion very highly, enhance the catalytic activity, and reduce the amount of catalyst to be used; mechanism of producing catalyst activating species to further enhance the activity of iron catalysts; and pursuit of morphological change in the activating species. The coal molecule scientific test and survey as the base for commercializing the coal liquefying technology performed the studies on the following items: pretreatment of coal that can realize reduction of coal liquefaction cost; configuration of the liquefaction reaction, liquefying catalysts, hydrocarbon gas generating mechanism, status of catalysts after liquefaction reaction, and reduction in gas purification cost by using gas separating membranes. Future possibilities were further searched through frank and constructive opinion exchanges among the committee members. (NEDO)

Two 3D structured Co-Ni bimetallic oxides as cathode catalysts for high-performance alkaline direct methanol fuel cells

Science.gov (United States)

Liu, Yan; Shu, Chengyong; Fang, Yuan; Chen, Yuanzhen; Liu, Yongning

2017-09-01

Two NiCo2O4 bimetallic oxides were synthesized via a facile hydrothermal method. SEM and TEM observations show that these materials have three-dimensional (3D) dandelion-like (DL) and flower-like (FL) morphologies. Their large specific surface areas (90.68 and 19.8 m2·g-1) and porous structures provide many active sites and effective transport pathways for the oxygen reduction reaction (ORR). Electrochemical measurements with a rotating ring-disc electrode (RRDE) indicate that the electron transfer numbers of the NiCo2O4-DL and NiCo2O4-FL catalysts for ORR in an alkaline solution are 3.97 and 3.91, respectively. Fuel cells were assembled with the bimetallic oxides, PtRu/C and a polymer fiber membrane (PFM) as cathode catalysts, anode catalyst and electrolyte film, respectively. For NiCo2O4-DL, the peak power density reaches up to 73.5 mW·cm-2 at 26 °C, which is the highest room-temperature value reported to date. The high catalytic activity of NiCo2O4 is mainly attributed to the presence of many Co3+ cations that directly donate electrons to O2 to reduce it via a more efficient and effective route. Furthermore, the catalytic performance of NiCo2O4-DL is superior to that of NiCo2O4-FL because it has a higher specific surface area and is less crystalline.

Small-sized and contacting Pt-WC nanostructures on graphene as highly efficient anode catalysts for direct methanol fuel cells.

Science.gov (United States)

Wang, Ruihong; Xie, Ying; Shi, Keying; Wang, Jianqiang; Tian, Chungui; Shen, Peikang; Fu, Honggang

2012-06-11

The synergistic effect between Pt and WC is beneficial for methanol electro-oxidation, and makes Pt-WC catalyst a promising anode candidate for the direct methanol fuel cell. This paper reports on the design and synthesis of small-sized and contacting Pt-WC nanostructures on graphene that bring the synergistic effect into full play. Firstly, DFT calculations show the existence of a strong covalent interaction between WC and graphene, which suggests great potential for anchoring WC on graphene with formation of small-sized, well-dispersed WC particles. The calculations also reveal that, when Pt attaches to the pre-existing WC/graphene hybrid, Pt particles preferentially grow on WC rather than graphene. Our experiments confirmed that highly disperse WC nanoparticles (ca. 5 nm) can indeed be anchored on graphene. Also, Pt particles 2-3 nm in size are well dispersed on WC/graphene hybrid and preferentially grow on WC grains, forming contacting Pt-WC nanostructures. These results are consistent with the theoretical findings. X-ray absorption fine structure spectroscopy further confirms the intimate contact between Pt and WC, and demonstrates that the presence of WC can facilitate the crystallinity of Pt particles. This new Pt-WC/graphene catalyst exhibits a high catalytic efficiency toward methanol oxidation, with a mass activity 1.98 and 4.52 times those of commercial PtRu/C and Pt/C catalysts, respectively. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Manganese Dioxide Coated Graphene Nanoribbons Supported Palladium Nanoparticles as an Efficient Catalyst for Ethanol Electrooxidation in Alkaline Media

International Nuclear Information System (INIS)

Liu, Qi; Jiang, Kun; Fan, Jinchen; Lin, Yan; Min, Yulin; Xu, Qunjie; Cai, Wen-Bin

2016-01-01

Design of appropriate supporting materials is an alternative route to yield efficient Pt-free catalysts for ethanol oxidation reaction, which in practice may determine the conversion efficiency of direct alkaline ethanol fuel cells. In this work, graphene nanoribbons (GNRs) coated with MnO_2 are used as a unique supporting material for loading and dispersing Pd nanoparticles. XRD, TEM and XPS are applied to characterize the structure of as-synthesized Pd/MnO_2/GNRs nanocomposite catalyst, revealing a good dispersion as well as a modification of electronic property of Pd nanoparticles. Electrochemical measurements demonstrate that the as-synthesized nanocomposite displays largely enhanced electrocatalytic activity and durability toward ethanol oxidation in alkaline media as compared to the other tested Pd-based catalysts with various supports.

Technology development for iron Fischer-Tropsch catalysts

Energy Technology Data Exchange (ETDEWEB)

O`Brien, R.J.; Raje, A.; Keogh, R.A. [and others

1995-12-31

The objective of this research project is to develop the technology for the production of physically robust iron-based Fischer-Tropsch catalysts that have suitable activity, selectivity and stability to be used in the slurry phase synthesis reactor development. The catalysts that are developed shall be suitable for testing in the Advanced Fuels Development Facility at LaPorte, Texas, to produce either low-or high-alpha product distributions. Previous work by the offeror has produced a catalyst formulation that is 1.5 times as active as the {open_quotes}standard-catalyst{close_quotes} developed by German workers for slurry phase synthesis. In parallel, work will be conducted to design a high-alpha iron catalyst this is suitable for slurry phase synthesis. Studies will be conducted to define the chemical phases present at various stages of the pretreatment and synthesis stages and to define the course of these changes. The oxidation/reduction cycles that are anticipated to occur in large, commercial reactors will be studied at the laboratory scale. Catalyst performance will be determined for catalysts synthesized in this program for activity, selectivity and aging characteristics.

A Comparative Characterization of the HPA-MCM-48 Type Catalysts Produced by the Direct Hydrothermal and Room Temperature Synthesis Methods

International Nuclear Information System (INIS)

Gucbilmez, Y.; Calis, I.; Yargic, A. S.

2012-01-01

MCM-48 type support materials synthesized by the direct hydrothermal synthesis (HTS) and room temperature synthesis (RTS) methods were incorporated with tungstophosphoric acid (TPA) in the range of 10-40 wt% by using a wet impregnation technique in methanol solutions. Resulting HPA-MCM-48 catalysts were characterized by the XRD, Nitrogen Physisorption, SEM, TEM, EDS, and FT-IR methods in order to determine the effects of different initial synthesis conditions on the catalyst properties. RTS samples were found to have better crystalline structures, higher BET surface areas, and higher BJH pore volumes than HTS samples. They also had slightly higher TPA incorporation, except for the 40 wt% samples, as evidenced by the EDS results. Keggin ion structure was preserved, for both methods, even at the highest acid loading of 40 wt%. It was concluded that the simpler and more economical RTS method was more successful than the HTS method for hetero poly acid incorporation into MCM-48 type materials

Minimizing Isolate Catalyst Motion in Metal-Assisted Chemical Etching for Deep Trenching of Silicon Nanohole Array.

Science.gov (United States)

Kong, Lingyu; Zhao, Yunshan; Dasgupta, Binayak; Ren, Yi; Hippalgaonkar, Kedar; Li, Xiuling; Chim, Wai Kin; Chiam, Sing Yang

2017-06-21

The instability of isolate catalysts during metal-assisted chemical etching is a major hindrance to achieve high aspect ratio structures in the vertical and directional etching of silicon (Si). In this work, we discussed and showed how isolate catalyst motion can be influenced and controlled by the semiconductor doping type and the oxidant concentration ratio. We propose that the triggering event in deviating isolate catalyst motion is brought about by unequal etch rates across the isolate catalyst. This triggering event is indirectly affected by the oxidant concentration ratio through the etching rates. While the triggering events are stochastic, the doping concentration of silicon offers a good control in minimizing isolate catalyst motion. The doping concentration affects the porosity at the etching front, and this directly affects the van der Waals (vdWs) forces between the metal catalyst and Si during etching. A reduction in the vdWs forces resulted in a lower bending torque that can prevent the straying of the isolate catalyst from its directional etching, in the event of unequal etch rates. The key understandings in isolate catalyst motion derived from this work allowed us to demonstrate the fabrication of large area and uniformly ordered sub-500 nm nanoholes array with an unprecedented high aspect ratio of ∼12.

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

Molecular Weight and Structural Properties of Biodegradable PLA Synthesized with Different Catalysts by Direct Melt Polycondensation

Directory of Open Access Journals (Sweden)

Hyung Woo Lee

2015-09-01

Full Text Available Production of biodegradable polylactic acid (PLA from biomassbased lactic acid is widely studied for substituting petro-based plastics or polymers. This study investigated PLA production from commercial lactic acid in a batch reactor by applying a direct melt polycondensation method with two kinds of catalyst, γ-aluminium(III oxide (γ-Al2O3 or zinc oxide (ZnO, in reduced pressure. The molecular weight of the synthesized PLA was determined by capillary viscometry and its structural properties were analyzed by functional group analysis using FT-IR. The yields of polymer production with respect to the theoretical conversion were 47% for γ-Al2O3 and 35% for ZnO. However, the PLA from ZnO had a higher molecular weight (150,600 g/mol than that from γ-Al2O3 (81,400 g/mol. The IR spectra of the synthesized PLA from both catalysts using polycondensation show the same behavior of absorption peaks at wave numbers from 4,500 cm-1 to 500 cm-1, whereas the PLA produced by two other polymerization methods – polycondensation and ring opening polymerization –showed a significant difference in % transmittance intensity pattern as well as peak area absorption at a wave number of 3,500 cm-1 as –OH vibration peak and at 1,750 cm-1 as –C=O carbonyl vibrational peak.

Energy conversion using Pt-Pd/C anode catalyst in direct 2-propanol fuel cell

Directory of Open Access Journals (Sweden)

S. S. Mahapatra

2016-06-01

Full Text Available The Pt-Pd/C electrocatalyst was synthesized on graphite substrate by the electrochemical codeposition technique. The Physico-chemical characterization of the catalyst was done by SEM, XRD and EDX. The electrochemical characterization of the Pt-Pd/C catalyst for 2-propanol electro-oxidation was studied over a range of 2-propanol concentrations in alkaline medium using cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy. The activity of 2-propanol oxidation increased with the increase of 2-propanol concentration, at 2-propanol concentration greater than 1.0 M, no change in the oxidation peak current density is because of excess 2-propanol at the electrode surface and/or depletion of OH− at the electrode surface. The Pt-Pd/C catalyst shows good stability and the low value of charge transfer resistance. The enhanced electrocatalytic activity of the electrodes is ascribed to the synergistic effect of higher electrochemical surface area, preferred OH− adsorption and ad-atom contribution on the alloyed surface.

Deactivation-resistant catalyst for selective catalyst reduction of NOx

DEFF Research Database (Denmark)

2011-01-01

The present invention relates to a catalyst for selective catalytic reduction of NOx in alkali metal containing flue gas using ammonia as reductant, the catalyst comprising a surface with catalytically active sites, wherein the surface is at least partly coated with a coating comprising at least...... one metal oxide. In another aspect the present invention relates to the use of said catalyst and to a method of producing said catalyst. In addition, the present invention relates to a method of treating an catalyst for conferring thereon an improved resistance to alkali poisoning....

Rapid and Efficient Collection of Platinum from Karstedt's Catalyst Solution via Ligands-Exchange-Induced Assembly.

Science.gov (United States)

Yang, Gonghua; Wei, Yanlong; Huang, Zhenzhu; Hu, Jiwen; Liu, Guojun; Ou, Ming; Lin, Shudong; Tu, Yuanyuan

2018-02-21

Reported herein is a novel strategy for the rapid and efficient collection of platinum from Karstedt's catalyst solution. By taking advantage of a ligand-exchange reaction between alkynols and the 1,3-divinyltetramethyldisiloxane ligand (M Vi M Vi ) that coordinated with platinum (Pt(0)), the Karstedt's catalyst particles with a size of approximately 2.5 ± 0.7 nm could be reconstructed and assembled into larger particles with a size of 150 ± 35 nm due to the hydrogen bonding between the hydroxyl groups of the alkynol. In addition, because the silicone-soluble M Vi M Vi ligand of the Karstedt's catalyst was replaced by water-soluble alkynol ligands, the resultant large particles were readily dispersed in water, resulting in rapid, efficient, and complete collection of platinum from the Karstedt's catalyst solutions with platinum concentrations in the range from ∼20 000 to 0.05 ppm. Our current strategy not only was used for the rapid and efficient collection of platinum from the Karstedt's catalyst solutions, but it also enabled the precise evaluation of the platinum content in the Karstedt's catalysts, even if this platinum content was extremely low (i.e., 0.05 ppm). Moreover, these platinum specimens that were efficiently collected from the Karstedt's catalyst solutions could be directly used for the evaluation of platinum without the need for pretreatment processes, such as calcination and digestion with hydrofluoric acid, that were traditionally used prior to testing via inductively coupled plasma mass spectrometry in conventional methods.

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%).

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)

Breaking the Fischer–Tropsch synthesis selectivity : Direct conversion of syngas to gasoline over hierarchical Co/H-ZSM-5 catalysts

NARCIS (Netherlands)

Sartipi, S.; Parashar, K.; Makkee, M.; Gascon, J.; Kapteijn, F.

2012-01-01

We report the combination of Fischer–Tropsch catalyst with acid functionality in one single catalyst particle. The resulting bifunctional catalyst is capable of producing gasoline range hydrocarbons from synthesis gas in one catalytic step with outstanding activities and selectivities.

The functionalities of Pt/{gamma}-Al{sub 2}O{sub 3} catalysts in simultaneous HDS and HDA reactions

Energy Technology Data Exchange (ETDEWEB)

V.G. Baldovino-Medrano; Sonia A. Giraldo; Aristobulo Centeno [Universidad Industrial de Santander (UIS), Bucaramanga (Colombia). Centro de Investigaciones en Catalisis (CICAT)

2008-08-15

A Pt/{gamma}-Al{sub 2}O{sub 3} catalyst was tested in simultaneous hydrodesulfurization (HDS) of dibenzothiophene and hydrodearomatization (HDA) of naphthalene reactions. Samples of it were subjected to different pretreatments: reduction, reduction-sulfidation, sulfidation with pure H{sub 2}S and non-activation. The reduced catalyst presented the best performance, even comparable to that of Co(Ni)Mo catalysts. All catalyst samples were selective to the HDS reaction over HDA, and to the direct desulfurization pathway of dibenzothiophene HDS over the hydrogenation reaction pathway of HDS. The effect of H{sub 2}S partial pressure on the functionalities of the reduced Pt/{gamma}-Al{sub 2}O{sub 3} catalyst was studied. The results showed that an increase in H{sub 2}S partial pressure does not cause poisoning, but an inhibition effect, without changing the catalyst selectivity. Accordingly, the activity trends were ascribed to adsorption differences between the different reactive molecules over the same catalytic active site. TPR characterization along with a thermodynamics analysis showed that the active phase of reduced Pt/{gamma}-Al{sub 2}O{sub 3} is constituted by Pt{sup 0} particles. However, presulfidation of the catalyst leads to a mixture of PtS and Pt{sup 0}which has a negative effect on the catalytic performance without changing catalyst functionalities. 61 refs., 4 figs., 1 tab.

Catalytic dehydration of ethanol using transition metal oxide catalysts.

Science.gov (United States)

Zaki, T

2005-04-15

The aim of this work is to study catalytic ethanol dehydration using different prepared catalysts, which include Fe(2)O(3), Mn(2)O(3), and calcined physical mixtures of both ferric and manganese oxides with alumina and/or silica gel. The physicochemical properties of these catalysts were investigated via X-ray powder diffraction (XRD), acidity measurement, and nitrogen adsorption-desorption at -196 degrees C. The catalytic activities of such catalysts were tested through conversion of ethanol at 200-500 degrees C using a catalytic flow system operated under atmospheric pressure. The results obtained indicated that the dehydration reaction on the catalyst relies on surface acidity, whereas the ethylene production selectivity depends on the catalyst chemical constituents.

Directed deposition of silicon nanowires using neopentasilane as precursor and gold as catalyst

Directory of Open Access Journals (Sweden)

Britta Kämpken

2012-07-01

Full Text Available In this work the applicability of neopentasilane (Si(SiH34 as a precursor for the formation of silicon nanowires by using gold nanoparticles as a catalyst has been explored. The growth proceeds via the formation of liquid gold/silicon alloy droplets, which excrete the silicon nanowires upon continued decomposition of the precursor. This mechanism determines the diameter of the Si nanowires. Different sources for the gold nanoparticles have been tested: the spontaneous dewetting of gold films, thermally annealed gold films, deposition of preformed gold nanoparticles, and the use of “liquid bright gold”, a material historically used for the gilding of porcelain and glass. The latter does not only form gold nanoparticles when deposited as a thin film and thermally annealed, but can also be patterned by using UV irradiation, providing access to laterally structured layers of silicon nanowires.

Vitrification of nanotoxic waste (Ru) from the production of nano-catalysts for direct ethanol fuel cells; Vitrificacao de nano-residuos toxicos (Ru) provenientes da producao de nano-catalisadores para celulas a combustivel de etanol direto

Energy Technology Data Exchange (ETDEWEB)

Silva, A.C.; Julio-Junior, O.; Mello-Castanho, S.R.H. [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil)

2010-07-01

Nanostructured catalysts have been developed for ethanol directly use in fuel cells, which due to the economic advantages that should have widespread use in the near future. The catalysts for these devices using nano-structured metal are based, where the toxic nature and environmental risks presented by these metals are largely enhanced by nano-dispersion. Thus, the production of nano-catalysts are potentially generating highly hazardous waste for public health and the environment. This study presents the treatment and inertization of ruthenium (Ru) nanoparticles waste containing by the vitrification technique and consequent attainment of silicate glasses for potential commercial use. Compositions were prepared containing up to about 20 wt % of nano-waste by changing the basic composition of glass soda-lime-borosilicate. After the fusion, at a temperature of 1100 deg C, the glasses were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and Infra-red in the Fourier transform (FT-IR) techniques. The chemical stability was evaluated by hydrolytic attack test. The glass containing 20 wt % of nano-residue showed a high chemical stability, similar to a usual soda-lime glass. (author)

Solid phosphoric acid oligomerisation: Manipulating diesel selectivity by controlling catalyst hydration

International Nuclear Information System (INIS)

Prinsloo, Nicolaas M.

2006-01-01

Solid phosphoric acid (SPA) catalyst is traditionally used in crude oil refineries to produce unhydrogenated motor-gasoline by propene and butene oligomerisation. SPA is also used in High-Temperature Fischer-Tropsch refineries (HTFT) to produce synthetic fuels albeit with a different emphasis. The petrol/diesel ratio of an HTFT refinery is very different from crude refining and it is often necessary to shift this ratio depending on market requirements. The influence of hydration was investigated as a means of improving diesel selectivity. This was achieved by studying SPA over a hydration range of 99-110% H 3 PO 4 , a temperature range of 140-230 o C and using C 3 -C 6 model and synthetic FT-derived olefinic feedstocks. A direct correlation was found between the selectivity towards diesel range products and the distribution of the phosphoric acid species viz. H 3 PO 4 , H 4 P 2 O 7 and H 5 P 3 O 10 . For various olefinic feedstocks, diesel selectivity increased with decreasing catalyst hydration with a maximum around 108% H 3 PO 4 for propene oligomerisation. Commercial tests confirmed the increase in diesel selectivity with lowered catalyst hydration. (author)

Electrochemical evaluation of Pt-Based binary catalysts on various supports for the direct methanol fuel cell

CSIR Research Space (South Africa)

Khotseng, L

2016-01-01

Full Text Available Ru/MoO(sub2) > PtSn/TiO(sub2) > PtRu/TiO(sub2). It was also observed that catalysts supported on MWCNTs were more active than those supported on metal oxides. Furthermore, catalysts supported on MWCNTs proved to be more stable than all the other supported...

In-situ environmental (scanning) transmission electron microscopy of catalysts at the atomic level

International Nuclear Information System (INIS)

Gai, P L; Boyes, E D

2014-01-01

Observing reacting single atoms on the solid catalyst surfaces under controlled reaction conditions is a key goal in understanding and controlling heterogeneous catalytic reactions. In-situ real time aberration corrected environmental (scanning) transmission electron microscopy (E(S)TEM permit the direct imaging of dynamic surface and sub-surface structures of reacting catalysts. In this paper in-situ AC ETEM and AC ESTEM studies under controlled reaction environments of oxide catalysts and supported metal nanocatalysts important in chemical industry are presented. They provide the direct evidence of dynamic processes at the oxide catalyst surface at the atomic scale and single atom dynamics in catalytic reactions. The ESTEM studies of single atom dynamics in controlled reaction environments show that nanoparticles act as reservoirs of ad-atoms. The results have important implications in catalysis and nanoparticle studies

Preparation of supported heterogeneous catalysts by pulse impregnation: Application to Ru[sub 3](CO)[sub 12]/2,2[prime]-bipyridine/SiO[sub 2] catalyst

Energy Technology Data Exchange (ETDEWEB)

Haukka, M.; Pakkanen, T.A. (Univ. of Joensuu (Finland))

1994-07-01

In this paper, the authors introduce pulse impregnation, a method for preparing supported heterogeneous catalysts by successive impregnation cycles. Pulse impregnation is a method for preparing supported heterogeneous catalysts from the liquid phase. In the pulse-impregnation technique the catalyst surface is grown gradually in consecutive cycles, with each cycle consisting of separate deposition and activation steps. During the deposition step, the catalyst precursor or precursors are deposited onto the support from a suitable solvent. The actual chemically bonded catalyst phase is formed during the activation step (e.g., thermal activation). Pulse impregnation was tested in the separate deposition of 2,2[prime]-bipyridine and Ru[sub 3](CO)[sub 12] onto a silica support, and in the preparation of Ru[sub 3](CO)[sub 12]/2,2[prime]-bipyridine/SiO[sub 2] catalyst, in a column-type reactor system. Macroscopically uniform deposition was achieved with both 2,2[prime]-bipyridine and Ru[sub 3](CO)[sub 12]. Various solvent systems were used to control the amount of solute adsorbed during deposition. In the preparation of the Ru[sub 3](CO)[sub 12]/2,2[prime]-bipyridine/SiO[sub 2] catalyst, the ruthenium content increased nearly linearly with the number of preparation cycles. The effects of the preparation method on the catalyst activity was also tested in 1-hexane hydroformylation. 31 refs., 7 figs., 1 tab.

Integrated test plan for directional boring

International Nuclear Information System (INIS)

Volk, B.W.

1993-01-01

This integrated test plan describes the field testing of the DITCH WITCH Directional Boring System. DITCH WITCH is a registered trademark of The Charles Machine Works, Inc., Perry, Oklahoma. The test is being conducted as a coordinated effort between Charles Machine Works (CMW), Sandia National Laboratories (SNL), and the Westinghouse Hanford Company (WHC). Funding for the WHC portion of the project is through the Volatile Organic Compound-Arid Integrated Demonstration (VOC-Arid ID). The purpose of the test is to evaluate the performance of the directional boring system for possible future use on environmental restoration projects at Hanford and other Department of Energy (DOE) sites. The test will be conducted near the 200 Areas Fire Station located between the 200 East and 200 West Area of the Hanford Site. The directional boring system will be used to drill and complete (with fiberglass casing) two horizontal boreholes. A third borehole will be drilled to test sampling equipment but will not be completed with casing

OPTIMATION OF TIME AND CATALYST/FEED RATIO IN CATALYTIC CRACKING OF WASTE PLASTICS FRACTION TO GASOLINE FRACTION USING Cr/NATURAL ZEOLITE CATALYST

Directory of Open Access Journals (Sweden)

Wega Trisunaryanti

2010-06-01

Full Text Available Optimation of time and catalyst/feed ratio in catalytic cracking of waste plastics fraction to gasoline fraction using Cr/Natural Zeolite catalyst has been studied.The natural zeolite was calcined by using nitrogen gas at 500 oC for 5 hours. The chromium supported on to the zeolite was prepared by ion exchange methode with Cr(NO33.9H2O solution with chromium/zeolite concentration of 1% (w/w. The zeolite samples were then calcined  with nitrogen gas at 500 oC for 2 hours, oxidyzed with oxygen gas and reduced with hydrogen at 400 oC for 2 hours. The characterization of the zeolite catalyst by means of Si/Al ratio by UV-Vis spectroscopy, acidity with pyridine vapour adsorption and Na, Ca and Cr contents by atomic adsorption spectroscopy (AAS. The catalyst activity test was carried out in the cracking process of waste plastics fraction with boiling point range of 150 - 250 °C (consisted of C12 - C16 hydrocarbons at 450 oC for 30 min, 60 min and 90 min, and catalyst/feed ratio 1/1, 1/2, 1/3, ¼ (w/w. The result of catalyst activity test  showed  that  the maximum number  conversion of gasoline fraction (C5-C11 is 53,27% with relatively low coke formation using 1/3 catalyst/feed ratio and the cracking time of 60 min.. This  catalyst has  Si/Al ratio = 1,21 (w/w , acidity = 0,16 mmol/g and Na content = 0,81%, Ca content = 0,15% and Cr content 0,24%.   Keywords: zeolite, catalytic cracking, gasoline, chromium.

New catalysts for exhaust gas cleaning

Energy Technology Data Exchange (ETDEWEB)

Haerkoenen, M [Kemira Metalkat Oy, Oulu (Finland)

1997-12-31

Major challenge for future catalyst systems was to develop thermally more stable washcoats for close coupled operating conditions and for engines operating under high speed and load conditions. To design these future emission systems extensive research and development was undertaken to develop methods to disperse and stabilize the key catalytic materials for operation at much higher temperatures. Second priority was to design catalysts that are more effective under low temperature exhaust conditions and have improved oxygen storage properties in the washcoats. Incorporating new materials and modified preparation technology a new generation of metallic catalyst formulations emerged, those being trimetallic K6 (Pt:Pd:Rh and bimetallic K7) (Pd+Pd:Rh). The target was to combine the best property of Pt:Rh (good NO{sub x} reduction) with that of the good HC oxidation activity of Pd and to ensure that precious metal/support interactions were positively maintained. Both K6 and K7 concepts contain special catalyst structures with optimized washcoat performance which can be brick converter configuration. Improvement in light-off, thermal stability and transient performance with these new catalyst formulations have clearly been shown in both laboratory and vehicle testing. (author) (20 refs.)

New catalysts for exhaust gas cleaning

Energy Technology Data Exchange (ETDEWEB)

Haerkoenen, M. [Kemira Metalkat Oy, Oulu (Finland)

1996-12-31

Major challenge for future catalyst systems was to develop thermally more stable washcoats for close coupled operating conditions and for engines operating under high speed and load conditions. To design these future emission systems extensive research and development was undertaken to develop methods to disperse and stabilize the key catalytic materials for operation at much higher temperatures. Second priority was to design catalysts that are more effective under low temperature exhaust conditions and have improved oxygen storage properties in the washcoats. Incorporating new materials and modified preparation technology a new generation of metallic catalyst formulations emerged, those being trimetallic K6 (Pt:Pd:Rh and bimetallic K7) (Pd+Pd:Rh). The target was to combine the best property of Pt:Rh (good NO{sub x} reduction) with that of the good HC oxidation activity of Pd and to ensure that precious metal/support interactions were positively maintained. Both K6 and K7 concepts contain special catalyst structures with optimized washcoat performance which can be brick converter configuration. Improvement in light-off, thermal stability and transient performance with these new catalyst formulations have clearly been shown in both laboratory and vehicle testing. (author) (20 refs.)

An introduction to catalyst

International Nuclear Information System (INIS)

Jeon, Hak Je

1988-11-01

This book explains basic conception of catalyst such as definition, velocity of chemical reaction and velocity of catalyst reaction, absorption with absorption energy and chemical absorption, pore structure with the role of pore and measurement of pore structure, catalyst activity on solid structure, electrical property on catalyst activity, choice and design of catalyst, catalytic reaction with reaction velocity and chemical equilibrium and reaction velocity model, measurement of reaction velocity and material analysis, catalyst for mixed compound, catalyst for solid acid and catalyst for supported metal.

Dehydration of alcohols using solid acid catalysts

OpenAIRE

Cholerton, Mary

2014-01-01

Solid acid catalysts were prepared through silicon substitution into aluminophosphate frameworks. Silicon incorporation was confirmed using solid state nuclear magnetic resonance spectroscopy. The nature of the acid sites generated was determined using Fourier Transform infrared spectroscopy. These materials were tested as catalysts for the dehydration of ethanol to ethylene at low operating temperatures. The materials were active for dehydration of ethanol to ethylene with significant differ...

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.

FY 1980 Report on results of Sunshine Project. Research and development of coal liquefaction techniques (Development of direct hydrogenation type liquefaction plant and researches on liquefaction reactions in the presence of iron-based catalyst); 1980 nendo sekitan ekika gijutsu no kenkyu kaihatsu, chokusetsu suiten ekika plant no kaihatsu seika hokokusho. Tetsukei shokubai ni yoru ekika hanno no kenkyu

Energy Technology Data Exchange (ETDEWEB)

NONE

1981-03-01

This program is aimed at development of iron-based catalyst suited for direct hydrogenation type coal liquefaction by elucidating the effects of the catalyst on the liquefaction reactions. The iron-based catalyst seems to act as the radical stabilizer rather than the reaction promoter, because the increased quantity of the catalyst and increased H{sub 2} pressure share the common pattern rather than the catalyst enhances the activity, which is associated with increased reaction temperature or residence time. This is more notably observed when the coal species is changed to brown coal. In other words, recombination of the decomposition products by polycondensation is accelerated in the presence of the catalyst in decomposition of brown coal from bituminous coal, with the result that the catalyst effects are more notably observed. Whether this results from difference in age between brown coal and bituminous coal or content of specific types of ashes should be elucidated, because this point is considered to deeply relate to eventual development of the liquefaction reaction system. The FY 1980 program includes the primary screening of different types of iron compounds and tests of some iron-metal-based catalysts. (NEDO)

Low Pt content Pt-Ru-Ir-Sn quaternary catalysts for anodic methanol oxidation in DMFC

Energy Technology Data Exchange (ETDEWEB)

Neburchilov, Vladimir; Wang, Haijiang; Zhang, Jiujun [Institute for Fuel Cell Innovation, National Research Council (Canada)

2007-07-15

In this communication we report our research work on low Pt content Pt-Ru-Ir-Sn quaternary catalysts for use in DMFC anodes. The carbon-supported quaternary metal alloy catalyst was synthesized according to the solution reduction method and was deposited onto a carbon fiber paper or a carbon aerogel nanofoam to form the anode for direct methanol fuel cells. The Pt loading of the electrode is 0.1 mg/cm{sup 2}. The testing results from a three-electrode electrochemical cell show that the simultaneous use of higher Ir (25-35 wt.%) and Sn (10 wt.%) content gives satisfactory stability and higher activity for methanol oxidation than the commercially available E-TEK anode (80%[0.5Pt 0.5Ru]/C on carbon cloth). Energy dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD), scanning electron microscope (SEM), and Bruner-Emmett-Teller method (BET) measurements were carried out to characterize the composition, structure, morphology, and surface area of the developed catalysts. (author)

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

Directory of Open Access Journals (Sweden)

Zhipeng Yu

2017-02-01

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

Low-Temperature Oxidation of Dimethyl Ether to Polyoxymethylene Dimethyl Ethers over CNT-Supported Rhenium Catalyst

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Qingde Zhang

2016-03-01

Full Text Available Due to its excellent conductivity, good thermal stability and large specific surface area, carbon nano-tubes (CNTs were selected as support to prepare a Re-based catalyst for dimethyl ether (DME direct oxidation to polyoxymethylene dimethyl ethers (DMMx. The catalyst performance was tested in a continuous flow type fixed-bed reactor. H3PW12O40 (PW12 was used to modify Re/CNTs to improve its activity and selectivity. The effects of PW12 content, reaction temperature, gas hourly space velocity (GHSV and reaction time on DME oxidation to DMMx were investigated. The results showed that modification of CNT-supported Re with 30% PW12 significantly increased the selectivity of DMM and DMM2 up to 59.0% from 6.6% with a DME conversion of 8.9%; besides that, there was no COx production observed in the reaction under the optimum conditions of 513 K and 1800 h−1. The techniques of XRD, BET, NH3-TPD, H2-TPR, XPS, TEM and SEM were used to characterize the structure, surface properties and morphology of the catalysts. The optimum amount of weak acid sites and redox sites promotes the synthesis of DMM and DMM2 from DME direct oxidation.

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

Science.gov (United States)

Workman, Michael J., Jr.

Fuel cells have the potential to be a pollution-free, low-cost, and energy efficient alternative to the internal combustion engine for transportation and small-scale stationary power applications. The current state of fuel cell technology has already achieved two of these three lofty goals. The remaining barrier to wide-scale deployment is the high cost, which is primarily caused by dependence on large amounts of platinum to catalyze the energy conversion reactions. To overcome this barrier and facilitate the integration of fuel cells into mainstream applications, research into a new class of catalyst materials that do not require platinum is needed. There has been a significant amount of research effort directed toward the development of platinum-group metal free (PGM-free) catalysts, yet there is a lack of consensus on both the engineering parameters necessary to improve the technology and the fundamental science that would facilitate rational design. I have engaged in research on PGM-free catalysts based on inexpensive and abundant reagents, specifically: nicarbazin and iron. Catalysts made from these precursors have previously proven to be among the best PGM-free catalysts, but their continued advancement suffered from the same lack of understanding that besets all catalysts in this class. The work I have performed address both engineering concerns and fundamental underlying principles. I present results demonstrating correlations between physical structure, chemical speciation, and synthesis parameters, as well as addressing active site chemistry and likely locations. My research presented herein introduces new morphology analysis techniques and elucidates several key structure-to-property characteristics of catalysts derived from iron and nicarbazin. I discuss the development and application of a new length-scale specific surface analysis technique that allows for analysis of well-defined size ranges from a few nm to several microns. The existing technique of

Potential for preparation of hot gas cleanup sorbents from spent hydroprocessing catalysts

Energy Technology Data Exchange (ETDEWEB)

Furimsky, E.; Biagini, M. [Canada Centre for Mineral and Energy Technology, Ottawa, ON (Canada). Energy Research Labs.

1996-01-01

Three spent-decoked hydroprocessing catalysts and two corresponding fresh catalysts were tested as hot gas clean-up sorbents and compared with the zinc ferrite using a simulated coal gasification gas mixture. The catalysts deposited only by coke exhibited relatively good cleaning efficiency. The catalyst deposited by coke and metals such as vanadium and nickel was less efficient. The useful life of the spent hydroprocessing catalysts may be extended if utilized as hot gas clean-up sorbents. 12 refs., 3 figs., 4 tabs.

Hydrogenation of toluene on Ni-Co-Mo supported zeolite catalysts ...

African Journals Online (AJOL)

-a, HY-b and Mordenite were prepared and characterized using many techniques for use as hydrotreating catalysts. In a preliminary investigation, toluene was employed as model compound to test the catalysts in hydrogenation, as a major ...

Comparison of sodium borohydride hydrolysis kinetics on Co-based nanocomposite catalysts

International Nuclear Information System (INIS)

Hristov, Georgi; Chorbadzhiyska, Elitsa; Mitov, Mario; Rashkov, Rashko; Hubenova, Yolina

2011-01-01

In this study, we compared the results, obtained with several Co-based nanocomposites (CoMnB, CoNiMnB and CoNiMoW) produced by electrodeposition on Ni-foam, as catalysts for the sodium borohydride hydrolysis reaction. Based on the comparative analyses, we propose CoNiMnB electrodeposits as most suitable catalysts for development of Hydrogen-on-Demand (HOD) system, while CoNiMoW ones as potential anodes for Direct Borohydride Fuel Cells (DBFCs). Keywords: Hydrogen-on-Demand (HOD), Nanocomposites, Hydrolysis, Catalyst, Kinetic

Shape-selective catalysts for Fischer-Tropsch chemistry. Final report: January 1, 2001 - December 31, 2008

International Nuclear Information System (INIS)

Cronauer, D.C.

2011-01-01

Argonne National Laboratory carried out a research program to create, prepare, and evaluate catalysts to promote Fischer-Tropsch (FT) chemistry-specifically, the reaction of hydrogen with carbon monoxide to form long-chain hydrocarbons. In addition to needing high activity, it was desirable that the catalysts have high selectivity and stability with respect to both mechanical strength and aging properties. It was desired that selectivity be directed toward producing diesel fraction components and avoiding excess yields of both light hydrocarbons and heavy waxes. The original goal was to produce shape-selective catalysts that had the potential to limit the formation of long-chain products and yet retain the active metal sites in a protected 'cage.' This cage would also restrict their loss by attrition during use in slurry-bed reactors. The first stage of this program was to prepare and evaluate iron-containing particulate catalysts. Such catalysts were prepared with silica-containing fractal cages. The activity and strength was essentially the same as that of catalysts without the cages. Since there was no improvement, the program plan was modified as discussed below. A second experimental stage was undertaken to prepare and evaluate active FT catalysts formed by atomic-layer deposition [ALD] of active components on supported membranes and particulate supports. The concept was that of depositing active metals (i.e. ruthenium, iron or cobalt) upon membranes with well defined flow channels of small diameter and length such that the catalytic activity and product molecular weight distribution could be controlled. In order to rapidly evaluate the catalytic membranes, the ALD coating processes were performed in an 'exploratory mode' in which ALD procedures from the literature appropriate for coating flat surfaces were applied to the high surface area membranes. Consequently, the Fe and Ru loadings in the membranes were likely to be smaller than those expected for

Sulphur poisoning of palladium catalysts used for methane combustion: Effect of the support

International Nuclear Information System (INIS)

Escandon, Lara S.; Ordonez, Salvador; Vega, Aurelio; Diez, Fernando V.

2008-01-01

Four different supported palladium catalysts (using alumina, silica, zirconia and titania as supports), prepared by incipient wetness impregnation, were tested as catalysts for methane oxidation in presence of sulphur dioxide. The catalyst supported on zirconia showed the best performance, whereas the silica-supported one showed the fastest deactivation. Temperature-programmed desorption experiments of the poisoned catalysts suggest that SO 2 adsorption capacity of the support plays a key role in the catalyst poisoning. In order to study the effect of promoters, expected to improve the thermal stability and thioresistance of the catalyst, commercial zirconia modified by yttrium and lantane was tested as supports. It was found that the presence of these promoters does not improve the performance of the zirconia-supported catalyst. A deactivation model - considering two different active sites (fresh and poisoning), pseudo-first order dependence on methane concentration and poisoning rate depending on sulphur concentration and fraction of non-poisoned palladium - was used for modelling the deactivation behaviour

Investigation of nano Pt and Pt-based alloys electrocatalysts for direct methanol fuel cells and their properties

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Chunguang Suo

2014-03-01

Full Text Available The electrocatalysts used in micro direct methanol fuel cell (μDMFC, such as Pt/C and Pt alloy/C, prepared by liquid-phase NaBH4 reduction method have been investigated. XC-72 (Cobalt corp. Company, U.S.A is chosen as the activated carrier for the electrocatalysts to keep the catalysts powder in the range of several nanometers. The XRD, SEM, EDX analyses indicated that the catalysts had small particle size in several nanometers, in excellent dispersed phase and the molar ratio of the precious metals was found to be optimal. The performances of the DMFCs using cathodic catalyst with Pt percentage of 30wt% and different anodic catalysts (Pt-Ru, Pt-Ru-Mo were tested. The polarization curves and power density curves of the cells were measured to determine the optimal alloy composition and condition for the electrocatalysts. The results showed that the micro direct methanol fuel cell with 30wt% Pt/C as the cathodic catalyst and n(Pt:n(Ru:n(Mo = 3:2:2 PtRuMo/C as the anodic catalyst at room temperature using 2.0mol/L methanol solution has the best performances.

Performance of a polymer electrolyte membrane fuel cell with thin film catalyst electrodes

Energy Technology Data Exchange (ETDEWEB)

Chun, Young Gab; Kim, Chang Soo; Peck, Dong Hyun; Shin, Dong Ryul [Korea Institute of Energy Research, Taejon (Korea, Republic of)

1998-03-15

In order to develop a kW-class polymer electrolyte membrane fuel cell (PEMFC), several electrodes have been fabricated by different catalyst layer preparation procedures and evaluated based on the cell performance. Conventional carbon paper and carbon cloth electrodes were fabricated using a ptfe-bonded Pt/C electrol catalyst by coating and rolling methods. Thin-film catalyst/ionomer composite layers were also formed on the membrane by direct coating and transfer printing techniques. The performance evaluation with catalyst layer preparation methods was carried out using a large or small electrode single cell. Conventional and thin film membrane and electrode assemblies (MEAs) with small electrode area showed a performance of 350 and 650 mA/cm{sup 2} at 0.6 V, respectively. The performance of direct coated thin film catalyst layer with 300 cm{sup 2} MEAs was higher than those of the conventional and transfer printing technique MEAs. The influence of some characteristic parameters of the thin film electrode on electrochemical performance was examined. Various other aspects of overall operation of PEMFC stacks were also discussed. (orig.)

Practical, economical, and eco-friendly starch-supported palladium catalyst for Suzuki coupling reactions.

Science.gov (United States)

Baran, Talat

2017-06-15

In catalytic systems, the support materials need to be both eco friendly and low cost as well as having high thermal and chemical stability. In this paper, a novel starch supported palladium catalyst, which had these outstanding properties, was designed and its catalytic activity was evaluated in a Suzuki coupling reaction under microwave heating with solvent-free and mild reaction conditions. The starch supported catalyst gave remarkable reaction yields after only 5min as a result of the coupling reaction of the phenyl boronic acid with 23 different substrates, which are bearing aril bromide, iodide, and chloride. The longevity of the catalyst was also investigated, and the catalyst could be reused for 10 runs. The starch supported Pd(II) catalyst yielded remarkable TON (up to 25,000) and TOF (up to 312,500) values by using a simple, fast and eco-friendly method. In addition, the catalytic performance of the catalyst was tested against different commercial palladium catalysts, and the green starch supported catalyst had excellent selectivity. The catalytic tests showed that the novel starch based palladium catalyst proved to be an economical and practical catalyst for the synthesis of biaryl compounds. Copyright © 2017 Elsevier Inc. All rights reserved.

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.

Hydrotreatment of heavy oil from coal liquefaction on Sulfide Ni - W Catalysts

International Nuclear Information System (INIS)

Zhi-ping Lei; Li-juan Gao; Heng-fu Shui; Shi-biao, Ren; Zhi-cai Wang; Kang-shi Gang

2011-01-01

Heavy oil (distillation temperature: 320-340 deg C) derived from the direct coal liquefaction process using Shengli coal were hydrotreated using sulfided Ni-Mo/Al 2 O 3 , Ni-W/Al 2 O 3 , and Ni-W/SiO 2 catalysts respectively. The sulfided catalysts were characterized by BET, XRD, H 2 -TPR and NH 3 -TPD respectively. The evaluations of the hydrodenitrogenation (HDN) and hydrodearomatization (HDA) properties of heavy oil on the three catalysts were carried out at 400 deg C and 5.0 MPa initial H2 pressure. The W-based catalysts displayed better performances than Mo-based catalysts for the HDN and HDA reactions. Al 2 O 3 supported catalysts were found to have higher catalytic activities than on SiO 2 supported ones. The activities of sulfided catalysts were associated mainly with the nature of active sites, acidity, metal sulfide crystallite size and the amount of the reducible sulfur species of metal sulfide. (author)

NO reduction by CO over noble-metal catalysts under cycled feedstreams

International Nuclear Information System (INIS)

Muraki, H.; Fujitani, Y.

1986-01-01

The reduction of NO with CO was studied over α-Al/sub 2/O/sub 3/-supported Pt, Pd, Rh, Ru, and Ir catalysts. The activities were measured by using cycled feeds and steady noncycled feed. The activity sequence of the catalysts tested was Rh > Ru > Ir > Pd > Pt. The activities of Pt and Pd catalysts were increased under the cycled feed. The periodic operation effect on the Pt catalyst was more predominant than that on the Pd catalyst. The order of periodic operation effect corresponded to the order of their susceptibility to CO self-poisoning

Controllable synthesis of SnO2 nanowires and nanobelts by Ga catalysts

International Nuclear Information System (INIS)

Xie Xing; Shao Zhibin; Yang Qianhui; Shen Xiaoshuang; Zhu Wei; Hong Xun; Wang Guanzhong

2012-01-01

We report the morphology control of one-dimensional (1D) SnO 2 nanostructures by Ga catalysts using thermal evaporation method. Gallium (Ga), either from decomposition of GaN powder or from Ga metal, is adopted as a catalyst for the growth of long SnO 2 nanowires and nanobelts. At similar experimental conditions, quantities of nanobelts are formed instead of nanowires when the temperature and reaction time are increased. Such approach enables us to synthesize various morphologies of SnO 2 nanobelts with different side facets. Novel nanobelts with [0 0 1] growth direction with high energy side facets are obtained for the first time, which is attributed to the large amount of oxygen vacancies introduced in the nanobelts by the Ga catalysts. - Graphical abstract: Morphology control of one-dimensional SnO 2 nanostructures are realized via a thermal evaporation method. Novel nanobelts along [0 0 1] direction having high energy side facets were fabricated for the first time. Highlights: ► Morphology control of one-dimensional SnO 2 nanostructures are realized by Ga catalysts using thermal evaporation method. ► Oxygen vacancies influenced the growth directions in order to neutralize thermodynamic instability. ► Novel nanobelts with [0 0 1] growth direction with high energy side facets are obtained for the first time.

Heterogeneous electro-Fenton catalyst for 1-butylpyridinium chloride degradation.

Science.gov (United States)

Meijide, Jessica; Pazos, Marta; Sanromán, Maria Ángeles

2017-10-15

The application of the electro-Fenton process for organic compound mineralisation has been widely reported over the past years. However, operational problems related to the use of soluble iron salt as a homogeneous catalyst involve the development of novel catalysts that are able to operate in a wide pH range. For this purpose, polyvinyl alcohol-alginate beads, containing goethite as iron, were synthesised and evaluated as heterogeneous electro-Fenton catalyst for 1-butylpyridinium chloride mineralisation. The influence of catalyst dosage and pH solution on ionic liquid degradation was analysed, achieving almost total oxidation after 60 min under optimal conditions (2 g/L catalyst concentration and pH 3). The results showed good catalyst stability and reusability, although its effectiveness decreases slightly after three successive cycles. Furthermore, a plausible mineralisation pathway was proposed based on the oxidation byproducts determined by chromatographic techniques. Finally, the Microtox® test revealed notable detoxification after treatment which demonstrates high catalyst ability for pyridinium-based ionic liquid degradation by the electro-Fenton process.

Enhanced gasification of wood in the presence of mixed catalysts

Energy Technology Data Exchange (ETDEWEB)

Weber, S. L.; Mudge, L. K.; Sealock, Jr., L. J.; Robertus, R. J.; Mitchell, D. E.

Experimental results obtained in laboratory investigations of steam gasification of wood in the presence of mixed catalysts are presented. These studies are designed to test the technical feasibility of producing specific gaseous products from wood by enhancing its reactivity and product specificity through the use of combined catalysts. The desired products include substitute natural gas, hydrocarbon synthesis gas and ammonia synthesis gas. The gasification reactions are controlled through the use of specific catalyst combinations and operating parameters. A primary alkali carbonate gasification catalyst impregnated into the wood combined with specific commercially available secondary catalysts produced the desired products. A yield of 50 vol % methane was obtained with a randomly mixed combination of a commercial nickel methanation catalyst and silica-alumina cracking catalyst at a weight ratio of 3:1 respectively. Steam gasification of wood in the presence of a commercial Si-Al cracking catalyst produced the desired hydrocarbon synthesis gas. Hydrogen-to-carbon monoxide ratios needed for Fischer-Tropsch synthesis of hydrocarbons were obtained with this catalyst system. A hydrogen-to-nitrogen ratio of 3:1 for ammonia synthesis gas was achieved with steam-air gasification of wood in the presence of catalysts. The most effective secondary catalyst system employed to produce the ammonia synthesis gas included two commercially prepared catalysts formulated to promote the water-gas shift reaction.

SEPARATION OF FISCHER-TROPSCH WAX PRODUCTS FROM ULTRAFINE IRON CATALYST PARTICLES

Energy Technology Data Exchange (ETDEWEB)

James K. Neathery; Gary Jacobs; Burtron H. Davis

2004-03-31

In this reporting period, a fundamental filtration study was started to investigate the separation of Fischer-Tropsch Synthesis (FTS) liquids from iron-based catalyst particles. Slurry-phase FTS in slurry bubble column reactor systems is the preferred mode of production since the reaction is highly exothermic. Consequently, heavy wax products must be separated from catalyst particles before being removed from the reactor system. Achieving an efficient wax product separation from iron-based catalysts is one of the most challenging technical problems associated with slurry-phase FTS. The separation problem is further compounded by catalyst particle attrition and the formation of ultra-fine iron carbide and/or carbon particles. Existing pilot-scale equipment was modified to include a filtration test apparatus. After undergoing an extensive plant shakedown period, filtration tests with cross-flow filter modules using simulant FTS wax slurry were conducted. The focus of these early tests was to find adequate mixtures of polyethylene wax to simulate FTS wax. Catalyst particle size analysis techniques were also developed. Initial analyses of the slurry and filter permeate particles will be used by the research team to design improved filter media and cleaning strategies.

The synthesis of nanostructured, phase pure catalysts by hydrodynamic cavitation

Energy Technology Data Exchange (ETDEWEB)

Moser, W.R.; Sunstrom, J.E.; Marshik-Geurts, B.J. [Worcester Polytechnic Institute, Worcester, MA (United States)

1995-12-01

A new process for the synthesis of advanced catalytic materials based on performing the synthesis under hydrodynamic cavitation conditions has been discovered. This continuous process for catalyst synthesis resulted in the formation of both supported and unsupported catalysts. The advantage of the process over classical methods of synthesis is that it permits the formation of a wide variety of nanostructured catalysts in exceptionally high phase purities. The synthesis of platinum and palladium catalysts supported on alumina and other supports resulted in high dispersions of the noble metals. The synthesis of alpha, beta- and gamma-bismuth molybdates resulted in catalysts having superior phase purities as compared to several other classical methods of synthesis. The beta-bismuth molybdate was synthesized directly onto Cabosil. These studies showed that the particle size of the active component could be varied from a few manometers to much larger grains. The process enabled the synthesis of other complex metal oxides like perovskites as pure phases. The process uses a commercially available Microfluidizer.

A comprehensive small and pilot-scale fixed-bed reactor approach for testing Fischer–Tropsch catalyst activity and performance on a BTL route

Directory of Open Access Journals (Sweden)

Piyapong Hunpinyo

2017-05-01

Full Text Available Ruthenium (Ru-based catalysts were prepared by the sol–gel technique for biomass-to-liquid (BTL operation and had their performance tested under different conditions. The catalytic study was carried out in two steps using a simple and reliable method. In the first step, the effects of reaction temperatures and inlet H2/CO molar feed ratios obtained from biomass gasification were investigated on the catalyst performance. A set of experimental results obtained in a laboratory fixed bed reactor was described and summarized. Moreover, a simplified Langmuir–Hinshelwood–Hougen–Watson (LHHW kinetic model was proposed with two promising models, where the surface decomposition of carbon monoxide was assumed as the rate determining step (RDS. In the second step, a FT pilot plant was conducted to validate the catalyst performance, especially the conversion efficiency, heat and mass transfer effects, and system controllability. The results indicated that our catalyst performances under mild conditions were not significantly different in many regards from those previously reported for a severe condition, as especially Ru-based catalyst can be performed to vary over a wide range of conditions to yield specific liquid productivity. The results in terms of the hydrocarbon product distribution obtained from the pilot scale operations were similar with that obtained from the related lab scale experiments.

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.

PREPARATION, CHARACTERIZATION, ACTIVITY, DEACTIVATION, AND REGENERATION TESTS OF CoO-MoO/ZnO AND CoO-MoO/ZnO-ACTIVATED ZEOLITE CATALYSTS FOR THE HYDROGEN PRODUCTION FROM FUSEL OIL

Directory of Open Access Journals (Sweden)

Wega Trisunaryanti

2010-06-01

Full Text Available Preparation, characterization, activation, deactivation, and regeneration tests of CoO-MoO/ZnO and CoO-MoO/ZnO-Activated Zeolite (AZ catalysts for the hydrogen production using steam reforming of alcohols in fusel oil have been conducted. Both catalysts were prepared by impregnation of Co and Mo onto ZnO or ZnO-AZ powder then followed by calcination at 400 °C for 5 h under N2 stream. The BET method and pyridine adsorption were used for catalysts characterization. The study of activation, deactivation, and regeneration of catalysts were conducted by using steam reforming method in the semi flow reactor. The reaction condition were: weight ratio of catalysts/feed = 0.1, temperature: 450 °C, duration: 45 min. The gas product was trapped in a 250 mL vacuum pyrex bottle filled with 50 mL of 4 M NaOH solution and analyzed by GC with TCD system to determine H2 existance and HCl titration to determine CO2 produced during the process that was dissolved in NaOH solution. The results showed that CoO-MoO/ZnO-AZ catalyst produced higher gas conversion than CoO-MoO/ZnO catalyst. However, it had short catalyst lifetime due to its high amount of coke deposited during the process. The regeneration test could enhance the catalyst activity. The gas product consisted of H2 (14.70% and CO2 (24.41%.   Keywords: fusel oil, steam reforming, deactivation, regeneration, hydrogen production.

Field-emission property of self-purification SiC/SiOx coaxial nanowires synthesized via direct microwave irradiation using iron-containing catalyst

Science.gov (United States)

Zhou, Qing; Yu, Yongzhi; Huang, Shan; Meng, Jiang; Wang, Jigang

2017-07-01

SiC/SiOx coaxial nanowires were rapidly synthesized via direct microwave irradiation in low vacuum atmosphere. During the preparation process, only graphite, silicon, silicon dioxide powders were used as raw materials and iron-containing substance was employed as catalyst. Comprehensive characterizations were employed to investigate the microstructure of the products. The results showed that a great quantity of coaxial nanowires with uniform sizes and high aspect ratio had been successfully achieved. The coaxial nanowires consist of a silicon oxide (SiOx) shell and a β-phase silicon carbide (β-SiC) core that exhibited in special tube brush like. In additional, nearly all the products were achieved in the statement of pure SiC/SiOx coaxial nanowires without the existence of metallic catalyst, indicating that the self-removal of iron (Fe) catalyst should be occurred during the synthesis process. Photoluminescence (PL) spectral analysis result indicated that such novel SiC/SiOx coaxial nanowires exhibited significant blue-shift. Besides, the measurement results of field-emission (FE) demonstrated that the SiC/SiOx coaxial nanowires had ultralow turn-on field and threshold field with values of 0.2 and 2.1 V/μm, respectively. The hetero-junction structure formed between SiOx shell and SiC core, lots of emission sites, as well as clear tips of the nanowires were applied to explain the excellent FE properties.[Figure not available: see fulltext.

Direct hydrodeoxygenation of cellulose and xylan to lower alkanes on ruthenium catalysts in subcritical water

International Nuclear Information System (INIS)

Osaka, Yuriko; Ikeda, Yoichi; Hashizume, Daisuke; Iwamoto, Masakazu

2013-01-01

Nano particles of Ru, Rh, Pd, Ir, Pt, and Au, protected by polyvinyl pyrrolidone (PVP), were applied to the hydrodeoxygenation of cellulose and xylan in water and 5 MPa H 2 at 543 K. The distributions of products generated from cellulose and xylan were roughly similar to each other under the present reaction conditions, and therefore, the former was intensively studied. The Ru-PVP catalyst afforded mainly methane and lower alkanes, rather than producing water soluble organic compounds, such as diols and alcohols, that were formed with the use of the other catalysts. The changes in the product distributions with reaction temperature and time indicated that the reaction consisted of two consecutive reactions: cellulose or xylan → water soluble compounds → hydrogenolysis. The first transformation was promoted in subcritical water, and the second step was catalyzed by the Ru catalyst. The Ru catalyst that was supported on CeO 2 , γ-Al 2 O 3 , or activated carbon yielded a similar product distribution to that on Ru-PVP; however, the loading of Ru on TiO 2 , ZrO 2 , SiO 2 –Al 2 O 3 , or SiO 2 resulted in the increment of diols. After the reaction a small portion of the CeO 2 and most of the SiO 2 –Al 2 O 3 and SiO 2 were dissolved in water, and a portion of the Al 2 O 3 was transformed to boehmite AlO(OH) from the γ-alumina. Little change in the catalytic activity however was observed upon the reuse of Ru/Al 2 O 3 in the second run. Highlights: •One-path hydrodeoxygenation of cellulose and xylan to methane and lower alkanes was studied. •Ru-PVP catalysts gave the best yields among Ru-, Rh-, Pd-, Ir-, Pt-, and Au-PVP. •The reaction pathways were cellulose → water soluble compounds → hydrogenolysis. •The catalytic activity of Ru was greatly dependent on the supports

The use of niobium based catalysts for liquid fuel production

Directory of Open Access Journals (Sweden)

Reguera Frank Martin

2004-01-01

Full Text Available The catalytic properties of niobium based catalysts were investigated in the conversion of oleic acid to liquid fuels at atmospheric pressure and at 623 K. The catalytic tests were performed in a fixed bed and continuous flow reactor using an acid to catalyst ratio equal to 4 and N2 as carrier gas. The reaction products were analyzed by gas chromatography and acidity measurements. NH3 temperature programmed desorption, N2 adsorption-desorption (BET method and Xray diffraction were also performed in order to determine the structural and acidic properties of the catalysts. From the catalytic tests, it was detected the formation of compounds in the range of gasoline, diesel and lubricant oils. Higher catalytic activity and selectivity for diesel fuel were observed for the catalysts NbOPO4 and H3PO4/Nb2O5 that possesses higher acidities and surface areas.

Magnetic nanoparticles conjugated to chiral imidazolidinone as recoverable catalyst

Energy Technology Data Exchange (ETDEWEB)

Mondini, Sara [Consiglio Nazionale delle Ricerche, Laboratorio di Nanotecnologie, Istituto di Scienze e Tecnologie Molecolari (Italy); Puglisi, Alessandra; Benaglia, Maurizio, E-mail: maurizio.benaglia@unimi.it; Ramella, Daniela [Università degli Studi di Milano, Dipartimento di Chimica (Italy); Drago, Carmelo [Consiglio Nazionale delle Ricerche, Istituto di Chimica Biomolecolare (Italy); Ferretti, Anna M.; Ponti, Alessandro, E-mail: alessandro.ponti@istm.cnr.it [Consiglio Nazionale delle Ricerche, Laboratorio di Nanotecnologie, Istituto di Scienze e Tecnologie Molecolari (Italy)

2013-11-15

The immobilization of an ad hoc designed chiral imidazolidin-4-one onto iron oxide magnetic nanoparticles (MNPs) is described, to afford MNP-supported MacMillan’s catalyst. Morphological and structural analysis of the materials, during preparation, use, and recycle, has been carried out by transmission electron microscopy. The supported catalyst was tested in the Diels–Alder reaction of cyclopentadiene with cinnamic aldehyde, affording the products in good yields and enantiomeric excesses up to 93 %, comparable to those observed with the non-supported catalyst. Recovery of the chiral catalyst has been successfully performed by simply applying an external magnet to achieve a perfect separation of the MNPs from the reaction product. The recycle of the catalytic system has been also investigated. Noteworthy, this immobilized MacMillan’s catalyst proved to be able to efficiently promote the reaction in pure water.

Magnetic nanoparticles conjugated to chiral imidazolidinone as recoverable catalyst

International Nuclear Information System (INIS)

Mondini, Sara; Puglisi, Alessandra; Benaglia, Maurizio; Ramella, Daniela; Drago, Carmelo; Ferretti, Anna M.; Ponti, Alessandro

2013-01-01

The immobilization of an ad hoc designed chiral imidazolidin-4-one onto iron oxide magnetic nanoparticles (MNPs) is described, to afford MNP-supported MacMillan’s catalyst. Morphological and structural analysis of the materials, during preparation, use, and recycle, has been carried out by transmission electron microscopy. The supported catalyst was tested in the Diels–Alder reaction of cyclopentadiene with cinnamic aldehyde, affording the products in good yields and enantiomeric excesses up to 93 %, comparable to those observed with the non-supported catalyst. Recovery of the chiral catalyst has been successfully performed by simply applying an external magnet to achieve a perfect separation of the MNPs from the reaction product. The recycle of the catalytic system has been also investigated. Noteworthy, this immobilized MacMillan’s catalyst proved to be able to efficiently promote the reaction in pure water

Nanostructured, mesoporous Au/TiO2 model catalysts – structure, stability and catalytic properties

Directory of Open Access Journals (Sweden)

Matthias Roos

2011-09-01

Full Text Available Aiming at model systems with close-to-realistic transport properties, we have prepared and studied planar Au/TiO2 thin-film model catalysts consisting of a thin mesoporous TiO2 film of 200–400 nm thickness with Au nanoparticles, with a mean particle size of ~2 nm diameter, homogeneously distributed therein. The systems were prepared by spin-coating of a mesoporous TiO2 film from solutions of ethanolic titanium tetraisopropoxide and Pluronic P123 on planar Si(100 substrates, calcination at 350 °C and subsequent Au loading by a deposition–precipitation procedure, followed by a final calcination step for catalyst activation. The structural and chemical properties of these model systems were characterized by X-ray diffraction (XRD, transmission electron microscopy (TEM, N2 adsorption, inductively coupled plasma ionization spectroscopy (ICP–OES and X-ray photoelectron spectroscopy (XPS. The catalytic properties were evaluated through the oxidation of CO as a test reaction, and reactivities were measured directly above the film with a scanning mass spectrometer. We can demonstrate that the thin-film model catalysts closely resemble dispersed Au/TiO2 supported catalysts in their characteristic structural and catalytic properties, and hence can be considered as suitable for catalytic model studies. The linear increase of the catalytic activity with film thickness indicates that transport limitations inside the Au/TiO2 film catalyst are negligible, i.e., below the detection limit.

MECHANISTIC STUDIES AND DESIGN OF HIGHLY ACTIVE CUPRATE CATALYSTS FOR THE DIRECT DECOMPOSITION AND SELECTIVE REDUCTION OF NITRIC OXIDE AND HYDROCARBONS TO NITROGEN FOR ABATEMENT OF STACK EMISSIONS

Energy Technology Data Exchange (ETDEWEB)

None

1998-04-30

A flow trough type catalytic reactor system was adequately modified for NO related catalytic and adsorption measurements, including the on-line connection of a digital chemiluminescent NO-NO{sub x} analyzer to the reactor outlet system. Moreover, we have largely completed the installation of an FTIR coupled catalytic system containing a HTEC cell for high temperature DRIFT studies. Three different barium cuprate samples, Ba{sub 2}CuO{sub 3}, BaCuO{sub 2}, and Ba{sub 2}Cu{sub 3}O{sub 5} were synthesized and characterized by powder XRD for catalytic tests. Prior to catalytic studies over these cuprates, a new, liquid indium based supported molten metal catalyst (In-SMMC) was tested in the reduction of NO by various reductants. In the presence of excess O{sub 2} and H{sub 2}O, the In-SMMC proved to be more active for the selective catalytic reduction (SCR) of NO to N{sub 2} by ethanol than most other catalysts. Using C{sub 1}-C{sub 3} alcohols as reductants, self sustained periodic oscillations observed in the NO{sub x} concentrations of reactor effluents indicated the first time that radical intermediates can be involved in the SCR of NO by alcohols. Further, In-SMMC is the only effective and water tolerant SCR catalyst reported thus far which contains SiO{sub 2} support. Thus, this novel catalyst opens up a promising new alternative for developing an effective and durable catalyst for NO{sub x} abatement in stack emission.

Recycling of waste spent catalyst in road construction and masonry blocks.

Science.gov (United States)

Taha, Ramzi; Al-Kamyani, Zahran; Al-Jabri, Khalifa; Baawain, Mahad; Al-Shamsi, Khalid

2012-08-30

Waste spent catalyst is generated in Oman as a result of the cracking process of petroleum oil in the Mina Al-Fahl and Sohar Refineries. The disposal of spent catalyst is of a major concern to oil refineries. Stabilized spent catalyst was evaluated for use in road construction as a whole replacement for crushed aggregates in the sub-base and base layers and as a partial replacement for Portland cement in masonry blocks manufacturing. Stabilization is necessary as the waste spent catalyst exists in a powder form and binders are needed to attain the necessary strength required to qualify its use in road construction. Raw spent catalyst was also blended with other virgin aggregates, as a sand or filler replacement, for use in road construction. Compaction, unconfined compressive strength and leaching tests were performed on the stabilized mixtures. For its use in masonry construction, blocks were tested for unconfined compressive strength at various curing periods. Results indicate that the spent catalyst has a promising potential for use in road construction and masonry blocks without causing any negative environmental impacts. Copyright © 2012 Elsevier B.V. All rights reserved.

Recombination Catalysts for Hypersonic Fuels

Science.gov (United States)

Chinitz, W.

1998-01-01

The goal of commercially-viable access to space will require technologies that reduce propulsion system weight and complexity, while extracting maximum energy from the products of combustion. This work is directed toward developing effective nozzle recombination catalysts for the supersonic and hypersonic aeropropulsion engines used to provide such access to space. Effective nozzle recombination will significantly reduce rk=le length (hence, propulsion system weight) and reduce fuel requirements, further decreasing the vehicle's gross lift-off weight. Two such catalysts have been identified in this work, barium and antimony compounds, by developing chemical kinetic reaction mechanisms for these materials and determining the engine performance enhancement for a typical flight trajectory. Significant performance improvements are indicated, using only 2% (mole or mass) of these compounds in the combustor product gas.

Design of an optimal micro direct methanol fuel cell for portable applications

International Nuclear Information System (INIS)

Ahmad, M.M.; Kamarudin, S.K.; Daud, W.R.W

2010-01-01

The main constraint for the commercialization of micro Direct Methanol Fuel cell (μDMFC) for small power generation is the performance of the fuel cell. In this study, a high-power μDMFC with a power output of 14.10 mW on an active area of 4 cm 2 and catalyst loading of 0.5 mg cm -2 cathode was successfully developed. The optimal parameters for methanol concentration and catalyst loading were determined. Besides that, testing of performance, long term and open circuit voltage (OCV) was also performed. (author)

Design of heterogeneous catalysts

DEFF Research Database (Denmark)

Frey, Anne Mette

was inspired by a computational screening, suggesting that alloys such as Ni-Fe, Co-Ni, and Co-Fe should show superior activity to the industrially used nickel catalyst. Especially the Ni-Fe system was considered to be interesting, since such alloy catalysts should be both more active and cheaper than the Ni...... catalyst. The results from the screening were experimentally verified for CO hydrogenation, CO2 hydrogenation, and simultaneous CO and CO2 hydrogenation by bimetallic Ni-Fe catalysts. These catalysts were found to be highly active and selective. The Co-Ni and Co-Fe systems were investigated for CO...... well, and the best catalyst prepared had a C5+ yield almost a factor of two higher than a standard air calcined Co catalyst. In the NH3-SCR reaction it is desirable to develop an active and stable catalyst for NOx removal in automotive applications, since the traditionally used vanadium-based catalyst...

Novel bimetallic dispersed catalysts for temperature-programmed coal liquefaction. Final report

Energy Technology Data Exchange (ETDEWEB)

Chunshan Song; Schobert, H.H.; Parfitt, D.P. [and others

1997-11-01

Development of new catalysts is a promising approach to more efficient coal liquefaction. It has been recognized that dispersed catalysts are superior to supported catalysts for primary liquefaction of coals, because the control of initial coal dissolution or depolymerization requires intimate contact between the catalyst and coal. This research is a fundamental and exploratory study on catalytic coal liquefaction, with the emphasis on exploring novel bimetallic dispersed catalysts for coal liquefaction and the effectiveness of temperature-programmed liquefaction using dispersed catalysts. The primary objective of this research was to explore novel bimetallic dispersed catalysts from organometallic molecular precursors, that could be used in low concentrations but exhibit relatively high activity for efficient hydroliquefaction of coals under temperature-programmed conditions. We have synthesized and tested various catalyst precursors in liquefaction of subbituminous and bituminous coals and in model compound studies to examine how do the composition and structure of the catalytic precursors affect their effectiveness for coal liquefaction under different reaction conditions, and how do these factors affect their catalytic functions for hydrogenation of polyaromatic hydrocarbons, for cleavage of C-C bonds in polycyclic systems such as 4-(1-naphthylmethyl)bibenzyl, for hydrogenolysis of C-O bond such as that in dinaphthylether, for hydrodeoxygenation of phenolic compounds and other oxygen-containing compounds such as xanthene, and for hydrodesulfurization of polycyclic sulfur compounds such as dibenzothiophene. The novel bimetallic and monometallic precursors synthesized and tested in this project include various Mo- and Fe-based compounds.

Plasma and catalyst for the oxidation of NOx

DEFF Research Database (Denmark)

Jögi, I.; Erme, K.; Levoll, E.

2017-01-01

The removal of NOx from the exhaust gases requires the oxidation of most abundant NO to NO2 or N2O5. The oxidation can be done by non-thermal plasma but the efficiency is limited due to the back-reaction of NO2 to NO by O radicals. Present contribution investigates the role of catalysts in the im......The removal of NOx from the exhaust gases requires the oxidation of most abundant NO to NO2 or N2O5. The oxidation can be done by non-thermal plasma but the efficiency is limited due to the back-reaction of NO2 to NO by O radicals. Present contribution investigates the role of catalysts...... in the improvement of oxidation efficiency based on the stationary and time-dependent studies of the NOx oxidation at different reactor configurations and experimental conditions. The plasma produced active oxygen species (O, O3) were shown to play an important role in the reactions taking place on the catalyst...... surfaces while the exact mechanism and extent of the effect depended on the reactor configuration. The effect of catalyst at different experimental conditions was quantitatively described with the aid of analytical lumped kinetic models derived for the NOx oxidation when the catalyst was directly...

Hydrotreatment of heavy oil from coal liquefaction on Sulfide Ni - W Catalysts

Energy Technology Data Exchange (ETDEWEB)

Zhi-ping Lei; Li-juan Gao; Heng-fu Shui; Shi-biao, Ren; Zhi-cai Wang; Kang-shi Gang, E-mail: shhf@ahut.edu.c [Anhui University of Technology, Maanshan (China). School of Chemistry and Chemical Engineering. Anhui Key Lab. of Coal Clean Conversion and Utilization

2011-07-01

Heavy oil (distillation temperature: 320-340 deg C) derived from the direct coal liquefaction process using Shengli coal were hydrotreated using sulfided Ni-Mo/Al{sub 2}O{sub 3}, Ni-W/Al{sub 2}O{sub 3}, and Ni-W/SiO{sub 2} catalysts respectively. The sulfided catalysts were characterized by BET, XRD, H{sub 2}-TPR and NH{sub 3}-TPD respectively. The evaluations of the hydrodenitrogenation (HDN) and hydrodearomatization (HDA) properties of heavy oil on the three catalysts were carried out at 400 deg C and 5.0 MPa initial H2 pressure. The W-based catalysts displayed better performances than Mo-based catalysts for the HDN and HDA reactions. Al{sub 2}O{sub 3} supported catalysts were found to have higher catalytic activities than on SiO{sub 2} supported ones. The activities of sulfided catalysts were associated mainly with the nature of active sites, acidity, metal sulfide crystallite size and the amount of the reducible sulfur species of metal sulfide. (author)

Highly dispersed metal catalyst

Science.gov (United States)

Xiao, Xin; West, William L.; Rhodes, William D.

2016-11-08

A supported catalyst having an atomic level single atom structure is provided such that substantially all the catalyst is available for catalytic function. A process of forming a single atom catalyst unto a porous catalyst support is also provided.

Catalytic cracking of iso-hexene over sapo-34 catalyst

International Nuclear Information System (INIS)

Nawaz, Z.; Shu, Q.

2009-01-01

The catalytic cracking of model feed compound, iso-hexene (2-methyl-1-pentene) was experimentally studied over 100% pure SAPO-34 zeolite catalyst. The critical focus was given to obtain maximum propylene selectivity. The product distributions were analyzed at temperature between 450-600 degree C. time-on-stream (TOS) from 1 to 5 min. and at WHSV = 7.9 h/sub -1/ The reaction behavior was quantified on both direct and indirect carbenium ion mechanisms owing to catalyst's small pore diameter with respect to 2-methyl-l-pentene kinetic diameter. The propylene yield and selectivity obtained was 41.2% and 43.1% respectively. with higher overall olefins selectivity 90.3%. The small pore size and week surface acid sites of 1000 percent pure SAPO-34 catalyst were found to be suitable for light olefins production and eliminate chances of bimolecular reactions. It was observed that both conversion and selectivity were strongly effected by TOS, as coke precursors become dominant and deactivate catalyst at higher TOS. (author)

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

Science.gov (United States)

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

2016-01-01

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

Current status for applications of hydrophobic platinum catalysts in tritium removal from nuclear effluents

International Nuclear Information System (INIS)

Vagner, Irina; Ionita, Gheorghe; Varlam, Carmen

2008-01-01

Full text: Based on the long experience of the authors, in the preparation, testing and evaluation of the performances of hydrophobic catalysts, and based on the reviewed references, this paper presents up-to-date R and D results on the preparation methods and applications of the hydrophobic catalysts, in deuterium and tritium separation. The objectives of the paper are: 1. to provide a database for selection of the most appropriate catalyst and catalytic packing for above mentioned processes; 2. to evaluate the potentiality of hydrophobic Pt-catalysts in the deuterium and tritium separation; 3. to assess and find a new procedure for preparation of a new improved hydrophobic catalyst. The merits of the hydrophobic catalysts are shown in comparison to hydrophilic catalysts. As results of the review some general conclusions about the applications of hydrophobic catalysts in environmental field are as follow: 1. the hydrophobic Pt-catalysts packed in the trickle bed reactors showed a high catalytic activity and long stability; 2. the utilization of the hydrophobic Pt-catalysts for tritium removal from liquid and gaseous effluent in nuclear field was entirely confirmed on industrial scale; 3. the extension of the utilization of the hydrophobic Pt-catalysts to other new processes, which take place in presence of liquid water or high humidity, like VOCs oxidation from wastewater or H 2 -O 2 catalytic recombination, are subject to testing

Development of catalysts for chemical reactions driven by concentrated solar energy

International Nuclear Information System (INIS)

Berman, A.; Levitan, R.; Levy, M.

1992-03-01

The aim of this phase of the work is to study commercially available low priced catalysts, for the methanation and reforming processes in the closed-loop solar chemical heat pipe. This report summarized some long term tests of commercially available methanation catalysts and the measurement of their active surface before and after reaction. It was found that the 1%Ru on alumina stars catalysts (prepared by Englehard Company according to our request) is very active and stable at 350-750 C. The catalyst 'A' produced in Russia, is less active, however, did not lose the mechanical strength. The 50% Ni/SiO 2 catalyst is active as the 'A' catalyst but loses its activity after treatment at temperature > 600 C, its geometrical size shrinked. (authors). 25 refs., 25 figs., 36 tabs

Properties and application of noble metal catalysts for heterogeneous catalytic hydrogenations

Energy Technology Data Exchange (ETDEWEB)

Horn, G; Frohning, C D; Cornils, B [Ruhrchemie A.G., Oberhausen (Germany, F.R.)

1976-07-01

The special properties of the six platinum group elements - ruthenium, rhodium, palladium, osmium, iridium, platinum - make them useful as active metals for catalytic reactions. Especially valuable is their property of favouring a single reaction even when the possibility of a number of parallel reactions exists under certain reaction conditions. This selectivity of the noble metal catalyst may be directed or enhanced through appropriate choise of the metal, the reaction conditions, the duration of the reaction, the amount of hydrogen etc. Even the physical state of the catalyst - supported or unsupported - is of influence when using noble metal catalysts as described in this report.

Basic study of catalyst aging in the H-coal process

Energy Technology Data Exchange (ETDEWEB)

Cable, T.L.; Massoth, F.E.; Thomas, M.G.

1985-04-01

Samples of CoMo/Al/sub 2/O/sub 3/ catalysts used in an H-coal process demonstration run were studied to determine causes of catalyst deactivation. Physical and surface properties of the aged and regenerated catalysts were examined. Model compounds were used to assess four catalyst activity functions, viz., hydrodesulfurization (HDS), hydrogenation, cracking and hydrodeoxygenation (HDO). Other tests were performed to study the effects of coke and metals separately on the four catalyst activity functions. Catalyst coke content and metal deposits first increased rapidly, then more gradually with exposure time in the process run. Surface area and pore volume markedly decreased with exposure time. Catalyst activities of aged catalysts showed a rapid decline with exposure time. One-day exposure to coal resulted in significant losses in HDS and hydrogenation activities and nearly complete loss in cracking and HDO activities. Although metal deposits caused some permanent catalyst deactivation, coke had a much greater effect. Regenerated catalysts showed less recovery of catalytic activity as processing time increased. These results agreed well with product inspections from the process run. Oxygen chemisorption on aged-regenerated catalysts decreased with catalyst exposure time, indicating a significant loss of active sites. However, ESCA results showed no evidence of extensive sintering of the active MoS/sub 2/ phase. Permanent deactivation of the longer-time exposed catalysts can be ascribed, at least partly, to lateral growth of the active molybdenum sulfide phase. In addition, some loss in cobalt promotion occurred early in the process, which may account for the rapid loss in HDS and HDO activity in regenerated catalysts. 24 references.

Industrial wastewater advanced treatment via catalytic ozonation with an Fe-based catalyst.

Science.gov (United States)

Li, Xufang; Chen, Weiyu; Ma, Luming; Wang, Hongwu; Fan, Jinhong

2018-03-01

An Fe-based catalyst was used as a heterogeneous catalyst for the ozonation of industrial wastewater, and key operational parameters (pH and catalyst dosage) were studied. The results indicated that the Fe-based catalyst significantly improved the mineralization of organic pollutants in wastewater. TOC (total organic carbon) removal was high, at 78.7%, with a catalyst concentration of 200 g/L, but only 31.6% with ozonation alone. The Fe-based catalyst significantly promoted ozone decomposition by 70% in aqueous solution. Hydroxyl radicals (·OH) were confirmed to be existed directly via EPR (electron paramagnetic resonance) experiments, and ·OH were verified to account for about 34.4% of TOC removal with NaHCO 3 as a radical scavenger. Through characterization by SEM-EDS (field emission scanning electron microscope with energy-dispersive spectrometer), XRD (X-ray powder diffraction) and XPS (X-ray photoelectron spectroscopy), it was deduced that FeOOH on the surface of the catalyst was the dominant contributor to the catalytic efficiency. The catalyst was certified as having good stability and excellent reusability based on 50 successive operations and could be used as a filler simultaneously. Thereby, it is a promising catalyst for practical industrial wastewater advanced treatment. Copyright © 2017 Elsevier Ltd. All rights reserved.

Shape-selective catalysts for Fischer-Tropsch chemistry. Final report : January 1, 2001 - December 31, 2008.

Energy Technology Data Exchange (ETDEWEB)

Cronauer, D. C. (Chemical Sciences and Engineering Division)

2011-04-11

Argonne National Laboratory carried out a research program to create, prepare, and evaluate catalysts to promote Fischer-Tropsch (FT) chemistry-specifically, the reaction of hydrogen with carbon monoxide to form long-chain hydrocarbons. In addition to needing high activity, it was desirable that the catalysts have high selectivity and stability with respect to both mechanical strength and aging properties. It was desired that selectivity be directed toward producing diesel fraction components and avoiding excess yields of both light hydrocarbons and heavy waxes. The original goal was to produce shape-selective catalysts that had the potential to limit the formation of long-chain products and yet retain the active metal sites in a protected 'cage.' This cage would also restrict their loss by attrition during use in slurry-bed reactors. The first stage of this program was to prepare and evaluate iron-containing particulate catalysts. Such catalysts were prepared with silica-containing fractal cages. The activity and strength was essentially the same as that of catalysts without the cages. Since there was no improvement, the program plan was modified as discussed below. A second experimental stage was undertaken to prepare and evaluate active FT catalysts formed by atomic-layer deposition [ALD] of active components on supported membranes and particulate supports. The concept was that of depositing active metals (i.e. ruthenium, iron or cobalt) upon membranes with well defined flow channels of small diameter and length such that the catalytic activity and product molecular weight distribution could be controlled. In order to rapidly evaluate the catalytic membranes, the ALD coating processes were performed in an 'exploratory mode' in which ALD procedures from the literature appropriate for coating flat surfaces were applied to the high surface area membranes. Consequently, the Fe and Ru loadings in the membranes were likely to be smaller than those

Toward Catalyst Design from Theoretical Calculations (464th Brookhaven Lecture)

Energy Technology Data Exchange (ETDEWEB)

Liu, Ping (BNL Chemistry Dept)

2010-12-15

Catalysts have been used to speed up chemical reactions as long as yeast has been used to make bread rise. Today, catalysts are used everywhere from home kitchens to industrial chemical factories. In the near future, new catalysts being developed at Brookhaven Lab may be used to speed us along our roads and highways as they play a major role in solving the world’s energy challenges. During the lecture, Liu will discuss how theorists and experimentalists at BNL are working together to formulate and test new catalysts that could be used in real-life applications, such as hydrogen-fuel cells that may one day power our cars and trucks.

Scalable synthesis of palladium nanoparticle catalysts by atomic layer deposition

International Nuclear Information System (INIS)

Liang Xinhua; Lyon, Lauren B.; Jiang Yingbing; Weimer, Alan W.

2012-01-01

Atomic layer deposition (ALD) was used to produce Pd/Al 2 O 3 catalysts using sequential exposures of Pd(II) hexafluoroacetylacetonate and formalin at 200 °C in a fluidized bed reactor. The ALD-prepared Pd/alumina catalysts were characterized by various methods including hydrogen chemisorption, XPS, and TEM, and compared with a commercially available 1 wt% Pd/alumina catalyst, which was also characterized. The content of Pd on alumina support and the size of Pd nanoparticles can be controlled by the number of ALD-coating cycles and the dose time of the Pd precursor. One layer of organic component from the Pd precursor remained on the Pd particle surface. The ALD 0.9 wt% Pd/alumina had greater active metal surface area and percent metal dispersion than the commercial 1 wt% Pd/alumina catalyst. The ALD and commercial catalysts were subjected to catalytic testing to determine their relative activities for glucose oxidation to gluconic acid in aqueous solution. The ALD 0.9 wt% Pd/alumina catalyst had comparable activity as compared to the commercial 1 wt% Pd catalyst. No noticeable amount of Pd leaching was observed for the ALD-prepared catalysts during the vigorously stirred reaction.

Study on the mechanism of a manganese-based catalyst for catalytic NOX flue gas denitration

Science.gov (United States)

Zhang, Lei; Wen, Xin; Lei, Zhang; Gao, Long; Sha, Xiangling; Ma, Zhenhua; He, Huibin; Wang, Yusu; Jia, Yang; Li, Yonghui

2018-04-01

Manganese-based bimetallic catalysts were prepared with self-made pyrolysis coke as carrier and its denitration performance of low-temperature SCR (selective catalyst reduction) was studied. The effects of different metal species, calcination temperature, calcination time and the metal load quantity on the denitration performance of the catalyst were studied by orthogonal test. The denitration mechanism of the catalyst was analyzed by XRD (X-ray diffraction), SEM (scanning electron microscope), BET test and transient test. The experiments show that: * The denitration efficiency of Mn-based bimetallic catalysts mainly relates to the metal type, the metal load quantity and the catalyst adjuvant type. * The optimal catalyst preparation conditions are as follows: the load quantity of monometallic MnO2 is 10%, calcined at 300°C for 4h, and then loaded with 8% CeO2, calcined at 350°Cfor 3h. * The denitration mechanism of manganese-based bimetallic oxide catalysts is stated as: NH3 is firstly adsorbed by B acid center Mn-OH which nears Mn4+==O to form NH4+, NH4+ was then attacked by the gas phase NO to form N2, H2O and Mn3+-OH. Finally, Mn3+-OH was oxidized by O2 to regenerate Mn4+.

Study on the mechanism of a manganese-based catalyst for catalytic NOX flue gas denitration

Directory of Open Access Journals (Sweden)

Lei Zhang

2018-04-01

Full Text Available Manganese-based bimetallic catalysts were prepared with self-made pyrolysis coke as carrier and its denitration performance of low-temperature SCR (selective catalyst reduction was studied. The effects of different metal species, calcination temperature, calcination time and the metal load quantity on the denitration performance of the catalyst were studied by orthogonal test. The denitration mechanism of the catalyst was analyzed by XRD (X-ray diffraction, SEM (scanning electron microscope, BET test and transient test. The experiments show that: ① The denitration efficiency of Mn-based bimetallic catalysts mainly relates to the metal type, the metal load quantity and the catalyst adjuvant type. ② The optimal catalyst preparation conditions are as follows: the load quantity of monometallic MnO2 is 10%, calcined at 300°C for 4h, and then loaded with 8% CeO2, calcined at 350°Cfor 3h. ③ The denitration mechanism of manganese-based bimetallic oxide catalysts is stated as: NH3 is firstly adsorbed by B acid center Mn-OH which nears Mn4+==O to form NH4+, NH4+ was then attacked by the gas phase NO to form N2, H2O and Mn3+-OH. Finally, Mn3+-OH was oxidized by O2 to regenerate Mn4+.

Effect of coke and catalyst structure on oxidative regeneration of hydroprocessing catalysts

Energy Technology Data Exchange (ETDEWEB)

Furimsky, E. (CANMET, Ottawa, ON (Canada). Energy Research Laboratories)

1991-04-01

Two industrial hydroprocessing catalysts used for upgrading an atmospheric residue and a gas oil, respectively were regenerated in a fixed bed using air and 2 vol.% O{sub 2}+N{sub 2} balance mixture. The regeneration in air resulted in a significant sintering of the catalyst's material. The surface area of catalysts regenerated in 2 vol.% O{sub 2} mixture was similar to that of fresh catalysts, whereas a significant loss of surface area was observed after regeneration in air. The X-ray diffraction pattern of catalysts regenerated in 2 vol.% O{sub 2}+N{sub 2} balance mixture was also similar to that of fresh catalysts. 22 refs., 9 figs., 7 tabs.

Determination of palladium, platinum and rhodium in used automobile catalysts and active pharmaceutical ingredients using high-resolution continuum source graphite furnace atomic absorption spectrometry and direct solid sample analysis

Energy Technology Data Exchange (ETDEWEB)

Resano, Martín, E-mail: mresano@unizar.es [Department of Analytical Chemistry, Aragón Institute of Engineering Research (I3A), University of Zaragoza, Pedro Cerbuna 12, 50009 Zaragoza (Spain); Flórez, María del Rosario [Department of Analytical Chemistry, Aragón Institute of Engineering Research (I3A), University of Zaragoza, Pedro Cerbuna 12, 50009 Zaragoza (Spain); Queralt, Ignasi [Institute of Earth Sciences Jaume Almera ICTJA-CSIC, Sole Sabarís s/n, 08028 Barcelona (Spain); Marguí, Eva [Department of Chemistry, Faculty of Sciences, Universitat de Girona, Campus Montilivi s/n, 17071 Girona (Spain)

2015-03-01

This work investigates the potential of high-resolution continuum source graphite furnace atomic absorption spectrometry for the direct determination of Pd, Pt and Rh in two samples of very different nature. While analysis of active pharmaceutical ingredients is straightforward and it is feasible to minimize matrix effects, to the point that calibration can be carried out against aqueous standard solutions, the analysis of used automobile catalysts is more challenging requiring the addition of a chemical modifier (NH{sub 4}F·HF) to help in releasing the analytes, a more vigorous temperature program and the use of a solid standard (CRM ERM®-EB504) for calibration. However, in both cases it was possible to obtain accurate results and precision values typically better than 10% RSD in a fast and simple way, while only two determinations are needed for the three analytes, since Pt and Rh can be simultaneously monitored in both types of samples. Overall, the methods proposed seem suited for the determination of these analytes in such types of samples, offering a greener and faster alternative that circumvents the traditional problems associated with sample digestion, requiring a small amount of sample only (0.05 mg per replicate for catalysts, and a few milligrams for the pharmaceuticals) and providing sufficient sensitivity to easily comply with regulations. The LODs achieved were 6.5 μg g{sup −1} (Pd), 8.3 μg g{sup −1} (Pt) and 9.3 μg g{sup −1} (Rh) for catalysts, which decreased to 0.08 μg g{sup −1} (Pd), 0.15 μg g{sup −1} (Pt) and 0.10 μg g{sup −1} (Rh) for pharmaceuticals. - Highlights: • Solid sampling HR CS GFAAS permits the fast and direct determination of Pd, Pt and Rh. • 2 determinations suffice for the 3 elements (2 of them can be measured simultaneously). • Samples as different as car catalysts and pharmaceuticals can be accurately analyzed. • Aqueous standards (pharmaceuticals) or a solid CRM (catalysts) is used for calibration. �

Atmosphere Processing Module Automation and Catalyst Durability Analysis for Mars ISRU Pathfinder

Science.gov (United States)

Petersen, Elspeth M.

2016-01-01

The Mars In-Situ Resource Utilization Pathfinder was designed to create fuel using components found in the planet’s atmosphere and regolith for an ascension vehicle to return a potential sample return or crew return vehicle from Mars. The Atmosphere Processing Module (APM), a subunit of the pathfinder, uses cryocoolers to isolate and collect carbon dioxide from Mars simulant gas. The carbon dioxide is fed with hydrogen into a Sabatier reactor where methane is produced. The APM is currently undergoing the final stages of testing at Kennedy Space Center prior to process integration testing with the other subunits of the pathfinder. The automation software for the APM cryocoolers was tested and found to perform nominally. The catalyst used for the Sabatier reactor was investigated to determine the factors contributing to catalyst failure. The results from the catalyst testing require further analysis, but it appears that the rapid change in temperature during reactor start up or the elevated operating temperature is responsible for the changes observed in the catalyst.

Pt-Pd bimetallic nanoparticles on MWCNTs: catalyst for hydrogen peroxide electrosynthesis

Energy Technology Data Exchange (ETDEWEB)

Felix-Navarro, R. M., E-mail: moi6salazar@hotmail.com; Beltran-Gastelum, M.; Salazar-Gastelum, M. I.; Silva-Carrillo, C.; Reynoso-Soto, E. A.; Perez-Sicairos, S.; Lin, S. W. [Centro de Graduados e Investigacion, Instituto Tecnologico de Tijuana (Mexico); Paraguay-Delgado, F. [Centro de Investigacion en Materiales Avanzados (Mexico); Alonso-Nunez, G. [Centro de Nanociencias y Nanotecnologia (Mexico)

2013-08-15

Bimetallic nanoparticles of Pt-Pd were deposited by the microemulsion method on a multiwall carbon nanotube (MWCNTs) to obtain a Pt-Pd/MWCNTs for electrocatalytic reduction of O{sub 2} to H{sub 2}O{sub 2}. The activity and selectivity of the catalyst was determined qualitatively by the rotating disk electrode method in acidic medium. The catalyst was spray-coated onto a reticulated vitreous carbon substrate and quantitatively was tested in bulk electrolysis for 20 min under potentiostatic conditions (0.5 V vs Ag/AgCl) in a 0.5 M H{sub 2}SO{sub 4} electrolyte using dissolved O{sub 2}. The bulk electrolysis experiments show that the Pt-Pd/MWCNTs catalyst is more efficient for H{sub 2}O{sub 2} electrogeneration than a MWCNTs catalyst. Nitrobenzene degradation by electrogenerated H{sub 2}O{sub 2} alone and Electro-Fenton process were also tested. Our results show that both processes decompose nitrobenzene, but the Electro-Fenton process does it more efficiently. The prepared nanoparticulated catalyst shows a great potential in environmental applications.

Productions of sunflower oil biodiesel and used cooking oil through heterogeneous catalysts compared to conventional homogeneous catalysts

International Nuclear Information System (INIS)

Gutiérrez-Zapata, C A; Collazos, C A; Acuña, H E Castellanos; Fernandez, C P; Martínez, D Blanco; Cuervo, J A

2017-01-01

This document compares homogeneous and heterogeneous catalysts used by production of biodiesel of sunflower oil and cooking oil used in frying. For this, NaOH was used as a catalyst homogeneous, and K 2 CO 3 and Na 2 CO 3 supported in gamma-alumina (K 2 CO 3 /γ Al 2 O 3 y Na 2 CO 3 /γ-Al 2 O 3 ) were synthesized as heterogeneous catalysts, which were characterized by X-ray diffraction. The transesterification tests were carried out for the sunflower oil and used cooking oil, in a reflux system, to different molar relations methanol/oil, depending on the type of oil and characterization of the same. The reflux system is performed at a temperature of 55-60°C for one hour. Finally, biofuel was characterized and the yield of the reaction was calculated. (paper)

Productions of sunflower oil biodiesel and used cooking oil through heterogeneous catalysts compared to conventional homogeneous catalysts

Science.gov (United States)

Gutiérrez-Zapata, C. A.; Blanco Martínez, D.; Collazos, C. A.; Castellanos Acuña, H. E.; Cuervo, J. A.; Fernandez, C. P.

2017-01-01

This document compares homogeneous and heterogeneous catalysts used by production of biodiesel of sunflower oil and cooking oil used in frying. For this, NaOH was used as a catalyst homogeneous, and K2CO3 and Na2CO3 supported in gamma-alumina (K2CO3/γ Al2O3 y Na2CO3 /γ-Al2O3) were synthesized as heterogeneous catalysts, which were characterized by X-ray diffraction. The transesterification tests were carried out for the sunflower oil and used cooking oil, in a reflux system, to different molar relations methanol/oil, depending on the type of oil and characterization of the same. The reflux system is performed at a temperature of 55-60°C for one hour. Finally, biofuel was characterized and the yield of the reaction was calculated.

Synthesis of CaO-CeO2 catalysts by soft template method for biodiesel production

Science.gov (United States)

Zheng, Y. C.; Yu, X. H.; Yang, J.

2017-06-01

Biodiesel has recently gained extensive attention. Catalysts play an important role in producing biodiesel by transesterification reaction. In this study, CaO-CeO2 catalysts are developed as the solid base catalyst. Using PDMS-PEO as a structure-directing agent, the prepared CaO-CeO2 catalysts have a three-dimensional interconnected porous structure, which benefits the transesterification reaction. While the added Ce slightly decreases the catalytic activity, the stability of the catalyst shows remarkable improvement. Considering the catalytic activity and stability, the best catalyst is determined to be catalyst 0.15-1073 (Ce/Ca molar ratio of 0.15 and calcination temperature of 1073 K). Under optimum reaction conditions, the biodiesel yield reaches to 97.5% and metal leaching is 117.7 ppm. For catalyst 0.15-1073 regenerated after four reaction cycles, the biodiesel yield is 94.1%. The results reveal that the CaO-CeO2 catalyst has good potential for application in large-scale biodiesel production in the future.

The effect of catalysts blending on coal pyrolysis

Energy Technology Data Exchange (ETDEWEB)

Pinto, F.; Gulyurtlu, I.; Lobo, L.S.; Cabrita, I. [INETI, Lisbon (Portugal)

1999-05-01

The effect of several catalysts on coal hydropyrolysis efficiency was studied, having selected catalysts with different characteristics and behaviours. For the experimental conditions used Fe{sub 2}O{sub 3} and ICI 41-6 showed selectivity towards lighter fractions, whilst ZnCl{sub 2} led to the highest coal conversion and to the greatest preasphaltenes yields. These results suggested the use of mixtures of catalysts. The heavier molecules of asphaltenes produced as a result of ZnCl{sub 2} action, could then be converted into lighter fractions by the action of a selective catalyst. Coal hydropyrolysis tests were undertaken using ZnCl{sub 2} mixed with Fe{sub 2}O{sub 3} or ICI 41-6. These mixtures of catalysts led to increased conversions and higher product yields. The best results were obtained in the presence of ZnCl{sub 2} mixed with Fe{sub 2}O{sub 3}. In an attempt to interpret these results, coal structure before and after swelling pre-treatment was also studied using SEM. 17 refs., 11 figs., 1 tab.

Use of Hydrogen Chemisorption and Ethylene Hydrogenation as Predictors for Aqueous Phase Reforming of Lactose over Ni@Pt and Co@Pt Bimetallic Overlayer Catalysts

Energy Technology Data Exchange (ETDEWEB)

Lai, Qinghua; Skoglund, Michael D.; Zhang, Chen; Morris, Allen R.; Holles, Joseph H.

2016-10-20

Overlayer Pt on Ni (Ni@Pt) or Co (Co@Pt) were synthesized and tested for H2 generation from APR of lactose. H2 chemisorption descriptor showed that Ni@Pt and Co@Pt overlayer catalysts had reduced H2 adsorption strength compared to a Pt only catalyst, which agree with computational predictions. The overlayer catalysts also demonstrated lower activity for ethylene hydrogenation than the Pt only catalyst, which likely resulted from decreased H2 binding strength decreasing the surface coverage of H2. XAS results showed that overlayer catalysts exhibited higher white line intensity than the Pt catalyst, which indicates a negative d-band shift for the Pt overlayer, further providing evidence for overlayer formation. Lactose APR studies showed that lactose can be used as feedstock to produce H2 and CO under desirable reaction conditions. The Pt active sites of Ni@Pt and Co@Pt overlayer catalysts showed significantly enhanced H2 production selectivity and activity when compared with that of a Pt only catalyst. The single deposition overlayer with the largest d-band shift showed the highest H2 activity. The results suggest that overlayer formation using directed deposition technique could modify the behavior of the surface metal and ultimately modify the APR activity.

Alkali/TX[sub 2] catalysts for CO/H[sub 2] conversion to C[sub 1]-C[sub 4] alcohols

Energy Technology Data Exchange (ETDEWEB)

Klier, K.; Herman, R.G.; Bastian, R.D.; Flanagan, K.L.

1989-01-01

Ruthenium disulfide catalysts have been synthesized, tested, and characterized during this period of research. It was observed that both the undoped and Cs-doped RuS[sub 2] catalysts produced alcohols and lower amounts of hydrocarbons from H[sub 2]/CO = 1.0 synthesis gas at temperatures above 300[degree]C. Calcination and catalytic testing resulted in partial reduction of the RuS[sub 2] to Ru[sup o]. Calcination under H[sub 2]S prevented the partial reduction of the RuS[sub 2] catalyst, but subsequent catalytic testing again resulted in the formation of a quantity of Ru[sup o]. A Cs-doped RuS[sub 2] catalyst was prepared, but it might have had too high of a loading of Cs. Upon testing, a lower activity was observed for the doped catalyst compared with the undoped catalyst, but the alcohol selectivity was the same for the two catalysts.

Photoassist-phosphorylated TiO2 as a catalyst for direct formation of 5-(hydroxymethyl)furfural from glucose.

Science.gov (United States)

Hattori, Masashi; Kamata, Keigo; Hara, Michikazu

2017-02-01

Photo-assisted phosphorylation of an anatase TiO 2 catalyst was examined to improve its catalytic performance for the direct production of 5-(hydroxymethyl)furfural (HMF), a versatile chemical platform, from glucose. In phosphorylation based on simple esterification between phosphoric acid and surface OH groups on anatase TiO 2 with water-tolerant Lewis acid sites, the density of phosphates immobilized on TiO 2 is limited to 2 phosphates nm -2 , which limits selective HMF production. Phosphorylation of the TiO 2 surface under fluorescent light irradiation increases the surface phosphate density to 50%, which is higher than the conventional limit, thus preventing the adsorption of hydrophilic glucose molecules on TiO 2 and resulting in a more selective HMF production over photoassist-phosphorylated TiO 2 .

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.

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.

New catalysts and new synthetic applications for hydroformylation

Energy Technology Data Exchange (ETDEWEB)

Breit, B. [Albert-Ludwigs-Univ. Freiburg (Germany). Inst. fuer Organische Chemie und Biochemie

2006-07-01

In the course of this lecture most recent advances in rhodium catalyzed hydroformylation and its use in organic synthesis are presented. Particular emphasis is given to regioselective hydroformylation of terminal alkenes and its application to fine chemical synthesis as well as latest results and applications of asymmetric hydroformylation. Furthermore, a new concept for simultaneous control of regio- and stereochemistry employing catalyst-directing groups will be discussed in detail. Finally, a new concept for catalyst library generation based on ligand-self-assembly through complementary hydrogen bonding and its application to regioselective hydroformylation as well as asymmetric hydrogenation is presented. (orig.)

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

International Nuclear Information System (INIS)

Galuh Widiyarti; Wuryaningsih Sri Rahayu

2010-01-01

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

Characterization and Regeneration of Pt-Catalysts Deactivated in Municipal Waste Flue Gas

DEFF Research Database (Denmark)

Rasmussen, Søren Birk; Kustov, Arkadii; Due-Hansen, Johannes

2006-01-01

Severe deactivation was observed for industrially aged catalysts used in waste incineration plants and tested in lab-scale. Possible compounds that cause deactivation of these Pt-based CO oxidation catalysts have been studied. Kinetic observations of industrial and model catalysts showed...... that siloxanes were the most severe catalyst poisons, although acidic sulfur compounds also caused deactivation. Furthermore, a method for on-site regeneration without shutdown of the catalytic flue gas cleaning system has been developed, i.e. an addition of H-2/N-2 gas to the off-gas can completely restore...... the activity of the deactivated catalysts. (c) 2006 Elsevier B.V. All rights reserved....

{alpha}-Al{sub 2}O{sub 3} catalyst supports for synthesis gas production: influence of different alumina bonding agents on support and catalyst properties

Energy Technology Data Exchange (ETDEWEB)

Marturano, M. [Centro de Investigacion y Desarrollo en Procesos Cataliticos, La Plata (Argentina); Aglietti, E.F. [Centro de Tecnologia de Recursos Minerales y Ceramica (CETMIC), Gonnet (Argentina); Ferretti, O. [Centro de Investigacion y Desarrollo en Procesos Cataliticos, La Plata (Argentina)]|[Univ. Nacional de La Plata, Dept. de Ingenieria Quimica de la Facultad de Ingenieria, La Plata (Argentina)

1997-02-01

Aluminas are widely used as catalytic supports in chemical reactions. Reforming reactions to obtain synthesis gas requires good mechanical strength and low sintering behaviour. In this work, the influence of bentonite, aluminium phosphate and alumina gel as binder agents of a calcined {alpha}-Al{sub 2}O{sub 3} are analyzed with respect to support and catalytic properties. The {alpha}-Al{sub 2}O{sub 3} supports, calcined at 1300 C, are then impregnated with solutions of Ni and Al inorganic salts to obtain the catalysts and are finally tested in the reforming reaction of methane to synthesis gas at 500-900 C. Supports and catalysts are characterized by XRD, SEM, N{sub 2} adsorption, mechanical strength test and other techniques. Mechanical strength depends on the type and quantity of binder material used during support preparation. The influence of the support on the performance of the resulting catalyst is evidenced by means of catalytic tests. (orig.) 8 refs.

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.

The generation of efficient supported (Heterogeneous) olefin metathesis catalysts

Energy Technology Data Exchange (ETDEWEB)

Grubbs, Robert H

2013-04-05

Over the past decade, a new family of homogeneous metathesis catalysts has been developed that will tolerate most organic functionalities as well as water and air. These homogeneous catalysts are finding numerous applications in the pharmaceutical industry as well as in the production of functional polymers. In addition the catalysts are being used to convert seed oils into products that can substitute for those that are now made from petroleum products. Seed oils are unsaturated, contain double bonds, and are a ready source of linear hydrocarbon fragments that are specifically functionalized. To increase the number of applications in the area of biomaterial conversion to petrol chemicals, the activity and efficiency of the catalysts need to be as high as possible. The higher the efficiency of the catalysts, the lower the cost of the conversion and a larger number of practical applications become available. Active supported catalysts were prepared and tested in the conversion of seed oils and other important starting materials. The outcome of the work was successful and the technology has been transferred to a commercial operation to develop viable applications of the discovered systems. A biorefinery that converts seed oils is under construction in Indonesia. The catalysts developed in this study will be considered for the next generation of operations.

Direction-Dependence Analysis: A Confirmatory Approach for Testing Directional Theories

Science.gov (United States)

Wiedermann, Wolfgang; von Eye, Alexander

2015-01-01

The concept of direction dependence has attracted growing attention due to its potential to help decide which of two competing linear regression models (X ? Y or Y ? X) is more likely to reflect the correct causal flow. Several tests have been proposed to evaluate hypotheses compatible with direction dependence. In this issue, Thoemmes (2015)…

Direct conversion of cellulose using carbon monoxide and water on a Pt-Mo2C/C catalyst

KAUST Repository

Li, Jing

2014-01-01

CO and H2O were employed as the hydrogen source for cellulose conversion to polyols. Pt-Mo2C/C tandem catalyst with the Pt-Mo 2C domain responsible for H2 and/or H production and the Pt-C domain for cellulose conversion was fabricated. Considerable polyols were obtained over this tandem Pt-Mo2C/C catalyst. This journal is © 2014 The Royal Society of Chemistry.

MAGNETO-CHEMICAL CHARACTER STUDIES OF NOVEL Fe CATALYSTS FOR COAL LIQUEFACTION

Energy Technology Data Exchange (ETDEWEB)

Murty A. Akundi; Jian H. Zhang; A.N. Murty; S.V. Naidu

2002-04-01

The objectives of the present study are: (1) To synthesize iron catalysts: Fe/MoO{sub 3}, and Fe/Co/MoO{sub 3} employing two distinct techniques: Pyrolysis with organic precursors and Co-precipitation of metal nitrates; (2) To investigate the magnetic character of the catalysts before and after exposure to CO and CO+H{sub 2} by (a) Mossbauer study of Iron (b) Zerofield Nuclear Magnetic Resonance study of Cobalt, and (c) Magnetic character of the catalyst composite; (3) To study the IR active surface species of the catalyst while stimulating (CO--Metal, (CO+H{sub 2})--Metal) interactions, by FTIR Spectroscopy; and (4) To analyze the catalytic character (conversion efficiency and product distribution) in both direct and indirect liquefaction Process and (5) To examine the correlations between the magnetic and chemical characteristics. This report presents the results of our investigation on (a) the effect of metal loading (b) the effect of intermetallic ratio and (c) the effect of catalyst preparation procedure on (i) the magnetic character of the catalyst composite (ii) the IR active surface species of the catalyst and (iii) the catalytic yields for three different metal loadings: 5%, 15%, and 25% (nominal) for three distinct intermetallic ratios (Fe/Co = 0.3, 1.5, 3.0).

Co-Production of Electricity and Hydrogen Using a Novel Iron-based Catalyst

Energy Technology Data Exchange (ETDEWEB)

Hilaly, Ahmad; Georgas, Adam; Leboreiro, Jose; Arora, Salil; Head, Megann; Trembly, Jason; Turk, Brian; Gupta, Raghubir

2011-09-30

The primary objective of this project was to develop a hydrogen production technology for gasification applications based on a circulating fluid-bed reactor and an attrition resistant iron catalyst. The work towards achieving this objective consisted of three key activities: Development of an iron-based catalyst suitable for a circulating fluid-bed reactor; Design, construction, and operation of a bench-scale circulating fluid-bed reactor system for hydrogen production; Techno-economic analysis of the steam-iron and the pressure swing adsorption hydrogen production processes. This report describes the work completed in each of these activities during this project. The catalyst development and testing program prepared and iron-based catalysts using different support and promoters to identify catalysts that had sufficient activity for cyclic reduction with syngas and steam oxidation and attrition resistance to enable use in a circulating fluid-bed reactor system. The best performing catalyst from this catalyst development program was produced by a commercial catalyst toll manufacturer to support the bench-scale testing activities. The reactor testing systems used during material development evaluated catalysts in a single fluid-bed reactor by cycling between reduction with syngas and oxidation with steam. The prototype SIP reactor system (PSRS) consisted of two circulating fluid-bed reactors with the iron catalyst being transferred between the two reactors. This design enabled demonstration of the technical feasibility of the combination of the circulating fluid-bed reactor system and the iron-based catalyst for commercial hydrogen production. The specific activities associated with this bench-scale circulating fluid-bed reactor systems that were completed in this project included design, construction, commissioning, and operation. The experimental portion of this project focused on technical demonstration of the performance of an iron-based catalyst and a

FY 1990 Study Meeting of Catalyst (Iron system). Data; 1990 nendo shokubai kento kai (Tetsu kei) shiryo

Energy Technology Data Exchange (ETDEWEB)

NONE

1991-03-01

The FY 1990 Study Meeting of Iron-system Catalyst was held at NEDO on March 12, 1991, and the data were arranged. In the study meeting, papers titled as follows were made public: About the behavior of H{sub 2}S on iron-system catalyst by Muroran Institute of Technology; Results of the test on iron-system catalyst in the BCL project by Research Institute, Mitsubishi Kasei Corp.; Results of the test on iron-system catalyst by 2.4 t/d PDU by NKK; Results of the test on iron-system catalyst by 0.1 t/d BSU by Mitsui Engineering and Shipbuilding Co.; Results of the test on iron-system catalyst by 1 t/d PSU by Nippon Steel Corp.; Results of the research at Government Industrial Development Laboratory, Hokkaido, and the study; Results of the research at National Chemical Laboratory for Industry and the study; Results of the research at the University of Tokyo and the study; Details of the development of synthetic iron sulfide and the attainment up to now by Asahi Chemical Industry Co. Moreover, the plenary session was held on research items for the development of iron-system catalyst in future. (NEDO)

Influence of Steam Reforming Catalyst Geometry on the Performance of Tubular Reformer – Simulation Calculations

Directory of Open Access Journals (Sweden)

Franczyk Ewelina

2015-06-01

Full Text Available A proper selection of steam reforming catalyst geometry has a direct effect on the efficiency and economy of hydrogen production from natural gas and is a very important technological and engineering issue in terms of process optimisation. This paper determines the influence of widely used seven-hole grain diameter (ranging from 11 to 21 mm, h/d (height/diameter ratio of catalyst grain and Sh/St (hole surface/total cylinder surface in cross-section ratio (ranging from 0.13 to 0.37 on the gas load of catalyst bed, gas flow resistance, maximum wall temperature and the risk of catalyst coking. Calculations were based on the one-dimensional pseudo-homogeneous model of a steam reforming tubular reactor, with catalyst parameters derived from our investigations. The process analysis shows that it is advantageous, along the whole reformer tube length, to apply catalyst forms of h/d = 1 ratio, relatively large dimensions, possibly high bed porosity and Sh/St ≈ 0.30-0.37 ratio. It enables a considerable process intensification and the processing of more natural gas at the same flow resistance, despite lower bed activity, without catalyst coking risk. Alternatively, plant pressure drop can be reduced maintaining the same gas load, which translates directly into diminishing the operating costs as a result of lowering power consumption for gas compression.

Preparation and performance of Pt/PTFE/Foam SiC as a hydrophobic catalyst for LPCE

International Nuclear Information System (INIS)

He, Jianchao; Wang, Heyi; Xiao, Chengjian; Li, Jiamao; Chen, Ping; Hou, Jingwei

2016-01-01

Highlights: • A new type of foam material, Foam SiC with three-dimensional network structure, was chosen as the carrier of catalyst. • Foam SiC was hydrophobic treated by PTFE, and achieved a good hydrophobic property. • Pt/PTFE/Foam SiC was prepared by impregnation method with Pt-organic solution and gaseous phase reduction method. • The hydrophobic catalysts were packed with Dixon phosphor bronze gauze rings (about 3 mm × 3 mm) in LPCE system to test the catalytic performance. • The effect of different size of the catalyst on LPCE was been tested. - Abstract: Platinum catalysts supported on a composite of polytetrafluoroethylene (PTFE) and Foam SiC (Pt/PTFE/Foam SiC) have been proposed and prepared by an impregnation method. The as-prepared Pt/PTFE/Foam SiC was characterized by compression load testing, dynamic contact angle measurement, SEM, XRD, and TEM. The results show that the catalyst prepared by triple hydrophobic treatment had an initial contact angle of 134.2°, a good compression performance of 3.2 MPa, and platinum nanoparticles of 12.1 nm (average size). The catalytic activity of the catalyst was tested with different packing methods, reaction temperatures, and gas-liquid ratios. An excellent hydrogen isotope exchange performance was observed using a hydrophilic packing material-to-catalyst ratio of 25% and reaction temperature of 80 °C. Pt/PTFE/Foam SiC may be used as a hydrophobic catalyst for a water detritiation system (WDS) via a liquid-phase catalytic exchange process (LPCE).

Preparation and performance of Pt/PTFE/Foam SiC as a hydrophobic catalyst for LPCE

Energy Technology Data Exchange (ETDEWEB)

He, Jianchao; Wang, Heyi, E-mail: hywang@caep.cn; Xiao, Chengjian; Li, Jiamao; Chen, Ping; Hou, Jingwei

2016-12-15

Highlights: • A new type of foam material, Foam SiC with three-dimensional network structure, was chosen as the carrier of catalyst. • Foam SiC was hydrophobic treated by PTFE, and achieved a good hydrophobic property. • Pt/PTFE/Foam SiC was prepared by impregnation method with Pt-organic solution and gaseous phase reduction method. • The hydrophobic catalysts were packed with Dixon phosphor bronze gauze rings (about 3 mm × 3 mm) in LPCE system to test the catalytic performance. • The effect of different size of the catalyst on LPCE was been tested. - Abstract: Platinum catalysts supported on a composite of polytetrafluoroethylene (PTFE) and Foam SiC (Pt/PTFE/Foam SiC) have been proposed and prepared by an impregnation method. The as-prepared Pt/PTFE/Foam SiC was characterized by compression load testing, dynamic contact angle measurement, SEM, XRD, and TEM. The results show that the catalyst prepared by triple hydrophobic treatment had an initial contact angle of 134.2°, a good compression performance of 3.2 MPa, and platinum nanoparticles of 12.1 nm (average size). The catalytic activity of the catalyst was tested with different packing methods, reaction temperatures, and gas-liquid ratios. An excellent hydrogen isotope exchange performance was observed using a hydrophilic packing material-to-catalyst ratio of 25% and reaction temperature of 80 °C. Pt/PTFE/Foam SiC may be used as a hydrophobic catalyst for a water detritiation system (WDS) via a liquid-phase catalytic exchange process (LPCE).

Utilization of a by-product produced from oxidative desulfurization process over Cs-mesoporous silica catalysts.

Science.gov (United States)

Kim, Hyeonjoo; Jeong, Kwang-Eun; Jeong, Soon-Yong; Park, Young-Kwon; Kim, Do Heui; Jeon, Jong-Ki

2011-02-01

We investigated the use of Cs-mesoporous silica catalysts to upgrade a by-product of oxidative desulfurization (ODS). Cs-mesoporous silica catalysts were characterized through N2 adsorption, XRD, CO2-temperature-programmed desorption, and XRF. Cs-mesoporous silica prepared by the direct incorporation method showed higher catalytic performance than a Cs/MCM-41 catalyst by impregnation method for the catalytic decomposition of sulfone compounds produced from ODS process.

Porous bimetallic PdNi catalyst with high electrocatalytic activity for ethanol electrooxidation.

Science.gov (United States)

Feng, Yue; Bin, Duan; Yan, Bo; Du, Yukou; Majima, Tetsuro; Zhou, Weiqiang

2017-05-01

Porous bimetallic PdNi catalysts were fabricated by a novel method, namely, reduction of Pd and Ni oxides prepared via calcining the complex chelate of PdNi-dimethylglyoxime (PdNi-dmg). The morphology and composition of the as-prepared PdNi were investigated by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD). Furthermore, the electrochemical properties of PdNi catalysts towards ethanol electrooxidation were also studied by electrochemical impedance spectrometry (EIS), cyclic voltammetry (CV) and chronoamperometry (CA) measurement. In comparison with porous Pd and commercial Pd/C catalysts, porous structural PdNi catalysts showed higher electrocatalytic activity and durability for ethanol electrooxidation, which may be ascribed to Pd and Ni property, large electroactive surface area and high electron transfer property. The Ni exist in the catalyst in the form of the nickel hydroxides (Ni(OH) 2 and NiOOH) which have a high electron and proton conductivity enhances the catalytic activity of the catalysts. All results highlight the great potential application of the calcination-reduction method for synthesizing high active porous PdNi catalysts in direct ethanol fuel cells. Copyright © 2017 Elsevier Inc. All rights reserved.

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

NARCIS (Netherlands)

Menon, P.G.; Prasad, J.

1970-01-01

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

Dispersed catalysts for co-processing and coal liquefaction

Energy Technology Data Exchange (ETDEWEB)

Bockrath, B.; Parfitt, D.; Miller, R. [Pittsburgh Energy Technology Center, PA (United States)

1995-12-31

The basic goal is to improve dispersed catalysts employed in the production of clean fuels from low value hydrocarbons. The immediate objective is to determine how the properties of the catalysts may be altered to match the demands placed on them by the properties of the feedstock, the qualities of the desired end products, and the economic constraints put upon the process. Several interrelated areas of the application of dispersed catalysts to co-processing and coal conversion are under investigation. The first involves control of the selectivity of MoS{sub 2} catalysts for HDN, HDS, and hydrogenation of aromatics. A second area of research is the development and use of methods to evaluate dispersed catalysts by means of activity and selectivity tests. A micro-flow reactor has been developed for determining intrinsic reactivities using model compounds, and will be used to compare catalysts prepared in different ways. Micro-autoclaves will also be used to develop data in batch experiments at higher partial pressures of hydrogen. The third area under investigation concerns hydrogen spillover reactions between MoS{sub 2} catalysts and carbonaceous supports. Preliminary results obtained by monitoring H{sub 2}/D{sub 2} exchange reactions with a pulse-flow microreactor indicate the presence of spillover between MoS{sub 2} and a graphitic carbon. A more complete study will be made at a later stage of the project. Accomplishments and conclusions are discussed.

The water gas shift reaction for automotive applications: preparation and testing of non pyrophoric copper catalysts

Energy Technology Data Exchange (ETDEWEB)

Quiney, A.S.; Germani, G.; Schuurman, Y.; Mirodatos, C. [Institut de Recherches sur la Catalyse - CNRS, 69 - Villeurbanne (France); Masset, A.S.F. [PSA Peugeot Citroen, 78 - Velizy Villacoublay (France)

2003-09-01

The aim of this study are: 1)to compare the performance of a non-pyrophoric catalyst (CuO/CeO{sub 2}/Al{sub 2}O{sub 3}) to that of a commercial copper catalyst (CuO/ZnO/Al{sub 2}O{sub 3}). 2)to develop a kinetic expression that fits the experimental data in order to design a WGS reactor. The comparison between the two catalysts shows that the latter (CuO/CeO{sub 2}/Al{sub 2}O{sub 3}) needs to be run at temperatures about 100 degrees Celsius higher. (O.M.)

Structural analysis of nickel doped cerium oxide catalysts for fuel reforming in solid oxide fuel cells

Science.gov (United States)

Cavendish, Rio

As world energy demands increase, research into more efficient energy production methods has become imperative. Heterogeneous catalysis and nanoscience are used to promote chemical transformations important for energy production. These concepts are important in solid oxide fuel cells (SOFCs) which have attracted attention because of their potential to provide an efficient and environmentally favorable power generation system. The SOFC is also fuel-flexible with the ability to run directly on many fuels other than hydrogen. Internal fuel reforming directly in the anode of the SOFC would greatly reduce the cost and complexity of the device. Methane is the simplest hydrocarbon and a main component in natural gas, making it useful when testing catalysts on the laboratory scale. Nickel (Ni) and gadolinium (Gd) doped ceria (CeO 2) catalysts for potential use in the SOFC anode were synthesized with a spray drying method and tested for catalytic performance using partial oxidation of methane and steam reforming. The relationships between catalytic performance and structure were then investigated using X-ray diffraction, transmission electron microscopy, and environmental transmission electron microscopy. The possibility of solid solutions, segregated phases, and surface layers of Ni were explored. Results for a 10 at.% Ni in CeO2 catalyst reveal a poor catalytic behavior while a 20 at.% Ni in CeO2 catalyst is shown to have superior activity. The inclusion of both 10 at.% Gd and 10 at.% Ni in CeO2 enhances the catalytic performance. Analysis of the presence of Ni in all 3 samples reveals Ni heterogeneity and little evidence for extensive solid solution doping. Ni is found in small domains throughout CeO2 particles. In the 20 at.% Ni sample a segregated, catalytically active NiO phase is observed. Overall, it is found that significant interaction between Ni and CeO2 occurs that could affect the synthesis and functionality of the SOFC anode.

A laboratory test setup for in situ measurements of the dielectric properties of catalyst powder samples under reaction conditions by microwave cavity perturbation: set up and initial tests.

Science.gov (United States)

Dietrich, Markus; Rauch, Dieter; Porch, Adrian; Moos, Ralf

2014-09-10

The catalytic behavior of zeolite catalysts for the ammonia-based selective catalytic reduction (SCR) of nitrogen oxides (NOX) depends strongly on the type of zeolite material. An essential precondition for SCR is a previous ammonia gas adsorption that occurs on acidic sites of the zeolite. In order to understand and develop SCR active materials, it is crucial to know the amount of sorbed ammonia under reaction conditions. To support classical temperature-programmed desorption (TPD) experiments, a correlation of the dielectric properties with the catalytic properties and the ammonia sorption under reaction conditions appears promising. In this work, a laboratory test setup, which enables direct measurements of the dielectric properties of catalytic powder samples under a defined gas atmosphere and temperature by microwave cavity perturbation, has been developed. Based on previous investigations and computational simulations, a resonator cavity and a heating system were designed, installed and characterized. The resonator cavity is designed to operate in its TM010 mode at 1.2 GHz. The first measurement of the ammonia loading of an H-ZSM-5 zeolite confirmed the operating performance of the test setup at constant temperatures of up to 300 °C. It showed how both real and imaginary parts of the relative complex permittivity are strongly correlated with the mass of stored ammonia.

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)

Formic acid oxidation at platinum-bismuth catalysts

Directory of Open Access Journals (Sweden)

Popović Ksenija Đ.

2015-01-01

Full Text Available The field of heterogeneous catalysis, specifically catalysis on bimetallic surfaces, has seen many advances over the past few decades. Bimetallic catalysts, which often show electronic and chemical properties that are distinct from those of their parent metals, offer the opportunity to obtain new catalysts with enhanced selectivity, activity, and stability. The oxidation of formic acid is of permanent interest as a model reaction for the mechanistic understanding of the electrooxidation of small organic molecules and because of its technical relevance for fuel cell applications. Platinum is one of the most commonly used catalysts for this reaction, despite the fact that it shows a few significant disadvantages: high cost and extreme susceptibility to poisoning by CO. To solve this problem, several approaches have been used, but generally, they all consist in the modification of platinum with a second element. Especially, bismuth has received significant attention as Pt modifier. According to the results presented in this survey dealing with the effects influencing the formic acid oxidation it was found that two types of Pt-Bi bimetallic catalysts (bulk and low loading deposits on GC showed superior catalytic activity in terms of the lower onset potential and oxidation current density, as well as exceptional stability compared to Pt. The findings in this report are important for the understanding of mechanism of formic acid electrooxidation on a bulk alloy and decorated surface, for the development of advanced anode catalysts for direct formic acid fuel cells, as well as for the synthesis of novel low-loading bimetallic catalysts. The use of bimetallic compounds as the anode catalysts is an effective solution to overcoming the problems of the formic acid oxidation current stability for long term applications. In the future, the tolerance of both CO poisoning and electrochemical leaching should be considered as the key factors in the development

Iron ore catalysts for methane decomposition to make CO x free hydrogen and carbon nano material

KAUST Repository

Zhou, Lu

2018-03-27

In this work, for the first time, iron ores with 91.7%–96.2% FeO, 1.3%–2.3% AlO, 1.2%–4.5% SiO, 1.3%–3.9% NaO, were studied directly as bulk catalysts for methane decomposition. By hydrogen pre-reduction at 850 °C, FeO species on iron ores were gradually reduced into FeO, FeO and then finally into Fe species. After reduction of 1.6 g of iron ore catalysts of 50 µm particle size with 100 mL/min pure H for 3.5 h at 850 °C, CMD life testing was conducted at 850 °C and GHSV of 3.75 L/g h and the catalyst showed a stable methane conversion for 5 h. When methane decomposition proceeded on Fe sites, FeC species would be formed to deposit graphite around themselves to finally form carbon nano onions. This carbon nano onions material showed excellent application for wastewater purification. All samples were fully characterized with XRF, XRD, H-TPR, TEM and Raman.

Catalytic Oxidation of Phenol over Zeolite Based Cu/Y-5 Catalyst: Part 1: Catalyst Preparation and Characterization

Directory of Open Access Journals (Sweden)

K. Maduna Valkaj

2015-01-01

Full Text Available The necessity to remove organic pollutants from the industrial wastewater streams has forced the development of new technologies that can produce better results in terms of pollutant removal and process efficiency in combination with low investment and operating costs. One of the new emerging processes with a potential to fulfil these demands is catalytic wet peroxide oxidation, commonly known as the CWPO process. The oxidative effect of the hydrogen peroxide is intensified by the addition of a heterogeneous catalyst that can reduce the operating conditions to atmospheric pressure and temperatures below 383 K. Zeolites, among others, are especially appealing as catalysts for selective oxidation processes due to their unique characteristics such as shape selectivity, thermal and chemical stability, and benign effect on nature and the living world. In this work, catalytic activity, selectivity and stability of Cu/Y-5 zeolite in phenol oxidation with hydrogen peroxide was examined. Catalyst samples were prepared by ion exchange method of the protonic form of commercial zeolite. The catalysts were characterized with powder X-ray diffraction (XRD, scanning electron microscopy (SEM, and AAS elemental analysis, while the adsorption techniques were used for the measurement of the specific surface area. The catalytic tests were carried out in a stainless steel Parr reactor in batch operation mode at the atmospheric pressure and in the temperature range from 323 to 353 K. The catalyst was prepared in powdered form and the mass fraction of the active metal component on the zeolite was 3.46 %. The initial concentration of phenol solution was equal to 0.01 mol dm−3 and the concentration of hydrogen peroxide ranged from 0.01 to 0.10 mol dm−3. The obtained experimental data was tested to a proposed kinetic model for phenol oxidation r = k1 cF cVP and hydrogen peroxide decomposition rHP = k2 cHP. The kinetic parameters were estimated using the Nelder

Development of Molecular Catalysts to Bridge the Gap between Heterogeneous and Homogeneous Catalysts

Science.gov (United States)

Ye, Rong

Catalysts, heterogeneous, homogeneous, and enzymatic, are comprised of nanometer-sized inorganic and/or organic components. They share molecular factors including charge, coordination, interatomic distance, bonding, and orientation of catalytically active atoms. By controlling the governing catalytic components and molecular factors, catalytic processes of a multichannel and multiproduct nature could be run in all three catalytic platforms to create unique end-products. Unifying the fields of catalysis is the key to achieving the goal of 100% selectivity in catalysis. Recyclable catalysts, especially those that display selective reactivity, are vital for the development of sustainable chemical processes. Among available catalyst platforms, heterogeneous catalysts are particularly well-disposed toward separation from the reaction mixture via filtration methods, which renders them readily recyclable. Furthermore, heterogeneous catalysts offer numerous handles - some without homogeneous analogues - for performance and selectivity optimization. These handles include nanoparticle size, pore profile of porous supports, surface ligands and interface with oxide supports, and flow rate through a solid catalyst bed. Despite these available handles, however, conventional heterogeneous catalysts are themselves often structurally heterogeneous compared to homogeneous catalysts, which complicates efforts to optimize and expand the scope of their reactivity and selectivity. Ongoing efforts are aimed to address the above challenge by heterogenizing homogeneous catalysts, which can be defined as the modification of homogeneous catalysts to render them in a separable (solid) phase from the starting materials and products. Specifically, we grow the small nanoclusters in dendrimers, a class of uniform polymers with the connectivity of fractal trees and generally radial symmetry. Thanks to their dense multivalency, shape persistence and structural uniformity, dendrimers have proven to

Communicating catalysts

Science.gov (United States)

Weckhuysen, Bert M.

2018-06-01

The beauty and activity of enzymes inspire chemists to tailor new and better non-biological catalysts. Now, a study reveals that the active sites within heterogeneous catalysts actively cooperate in a fashion phenomenologically similar to, but mechanistically distinct, from enzymes.

A biomimetic methane-oxidising catalyst

Energy Technology Data Exchange (ETDEWEB)

Dalton, H [Warwick Univ., Coventry (United Kingdom). Dept. of Biological Sciences

1997-12-31

The diminishing resources of petroleum oil has meant that there has been considerable efforts in recent years to find a suitable substitute for gasoline as a transportation fuel. Methanol has been identified as a suitable substitute since it is a readily combustible fuel which can be manufactured from a number of different sources. Methane is commonly used as a starting material for the production of synthesis gas (CO + H{sub 2}) and hence methanol. It is well known that the cleavage of the C-H bond of methane is extremely difficult (bond energy is around 104 kcal/mol) and that fairly drastic conditions are required to convert methane into methanol. Temperatures around 1200 deg C and pressures of up to 100 atmospheres over metal catalysts in a series of reactions are required to effect this process. Efforts have been made to reduce the temperature and the number of steps by using lanthanide ruthenium oxide catalyst but such reactions are still thermodynamically endothermic. An energetically more efficient reaction would be the direct conversion of methane to methanol using oxygen as the oxidant: CH{sub 4} + 1/2O{sub 2} -> CH{sub 3}OH {Delta}H deg = - 30.7 kcal/mol. Such a direct oxidation route is manifest in the bacterially-mediated oxidation of methane by methanotrophic bacteria. These organisms effect the direct oxidation of methane to methanol by the enzyme methane monooxygenase (MMO) as part of the reaction sequences to oxidize methane to carbon dioxide. (14 refs.)

A biomimetic methane-oxidising catalyst

Energy Technology Data Exchange (ETDEWEB)

Dalton, H. [Warwick Univ., Coventry (United Kingdom). Dept. of Biological Sciences

1996-12-31

The diminishing resources of petroleum oil has meant that there has been considerable efforts in recent years to find a suitable substitute for gasoline as a transportation fuel. Methanol has been identified as a suitable substitute since it is a readily combustible fuel which can be manufactured from a number of different sources. Methane is commonly used as a starting material for the production of synthesis gas (CO + H{sub 2}) and hence methanol. It is well known that the cleavage of the C-H bond of methane is extremely difficult (bond energy is around 104 kcal/mol) and that fairly drastic conditions are required to convert methane into methanol. Temperatures around 1200 deg C and pressures of up to 100 atmospheres over metal catalysts in a series of reactions are required to effect this process. Efforts have been made to reduce the temperature and the number of steps by using lanthanide ruthenium oxide catalyst but such reactions are still thermodynamically endothermic. An energetically more efficient reaction would be the direct conversion of methane to methanol using oxygen as the oxidant: CH{sub 4} + 1/2O{sub 2} -> CH{sub 3}OH {Delta}H deg = - 30.7 kcal/mol. Such a direct oxidation route is manifest in the bacterially-mediated oxidation of methane by methanotrophic bacteria. These organisms effect the direct oxidation of methane to methanol by the enzyme methane monooxygenase (MMO) as part of the reaction sequences to oxidize methane to carbon dioxide. (14 refs.)

Direct catalytic conversion of brown seaweed-derived alginic acid to furfural using 12-tungstophosphoric acid catalyst in tetrahydrofuran/water co-solvent

International Nuclear Information System (INIS)

Park, Geonu; Jeon, Wonjin; Ban, Chunghyeon; Woo, Hee Chul; Kim, Do Heui

2016-01-01

Highlights: • Furfural was produced by catalytic conversion of macroalgae-derived alginic acid. • 12-Tungstophosphoric acid (H_3PW_1_2O_4_0) showed remarkable catalytic performance. • Tetrahydrofuran (THF) as a reaction medium significantly enhanced production of furfural. - Abstract: Furfural, a biomass-derived platform chemical, was produced by acid-catalyzed reaction of alginic acid extracted from brown seaweed. Three acid catalysts, H_2SO_4, Amberlyst15 and 12-tungstophosphoric acid (H_3PW_1_2O_4_0), were compared to evaluate their catalytic performance for the alginic acid conversion. The H_3PW_1_2O_4_0 catalyst showed the highest catalytic activity, yielding the maximum furfural yield (33.8%) at 180 °C for 30 min in tetrahydrofuran/water co-solvent. Higher reaction temperature promoted the conversion of alginic acid to furfural, but the transformation of furfural to humin was also accelerated. To our knowledge, this is the highest furfural yield among studies about the direct catalytic conversion of alginic acid. Furthermore, products distribution with time-on-stream was investigated in detail, which led us to propose a reaction pathway.

Methods of making textured catalysts

Science.gov (United States)

Werpy, Todd [West Richland, WA; Frye, Jr., John G.; Wang, Yong [Richland, WA; Zacher, Alan H [Kennewick, WA

2010-08-17

A textured catalyst having a hydrothermally-stable support, a metal oxide and a catalyst component is described. Methods of conducting aqueous phase reactions that are catalyzed by a textured catalyst are also described. The invention also provides methods of making textured catalysts and methods of making chemical products using a textured catalyst.

Synthesis of novel perfluoroalkylglucosides on zeolite and non-zeolite catalysts.

Science.gov (United States)

Nowicki, Janusz; Mokrzycki, Łukasz; Sulikowski, Bogdan

2015-04-08

Perfluoroalkylglucosides comprise a very important class of fluorine-containing surfactants. These compounds can be synthesized by using the Fisher reaction, starting directly from glucose and the required perfluoroalcohols. We wish to report on the use of zeolite catalysts of different structure and composition for the synthesis of perfluoroalkylglucosides when using glucose and 1-octafluoropentanol as substrates. Zeolites of different pore architecture have been chosen (ZSM-5, ZSM-12, MCM-22 and Beta). Zeolites were characterized by XRD, nitrogen sorption, scanning electron microscopy (SEM) and solid-state 27Al MAS NMR spectroscopy. The activity of the zeolite catalysts in the glycosidation reaction was studied in a batch reactor at 100 °C below atmospheric pressure. The performance of zeolites was compared to other catalysts, an ion-exchange resin (Purolite) and a montmorillonite-type layered aluminosilicate. The catalytic performance of zeolite Beta was the highest among the zeolites studied and the results were comparable to those obtained over Purolite and montmorillonite type catalysts.

Porous-microelectrode study on Pt/C catalysts for methanol electrooxidation

International Nuclear Information System (INIS)

Umeda, Minoru; Kokubo, Mitsuhiro; Mohamedi, Mohamed; Uchida, Isamu

2003-01-01

We have developed a porous-microelectrode (PME) to investigate the electroactivity of catalyst particles for proton exchange membrane fuel cells. The cavity at the tip of the PME was filled with Pt/C catalysts prepared by impregnation method. Cyclic voltammograms (CVs) recorded in 1 N H 2 SO 4 aqueous solution revealed that the active area of the stacked catalysts exist not only at the surface but also inside of the stack. For methanol electrooxidation, 30 wt.% Pt/C exhibited the highest electroactivity, whereas the 50 wt.% Pt/C showed extremely small current. The small current is considered as a result of a small active-surface area. Methanol oxidation peak potential shifted toward cathodic direction as Pt-loading decreased, which agrees well with the Pt-oxide formation potential. The activation energy for methanol oxidation was assessed to be 44±3 kJ mol -1 for all Pt/C catalysts and Pt-disc electrode

Oxidation Catalysts for Elemental Mercury in Flue Gases—A Review

Directory of Open Access Journals (Sweden)

Liliana Lazar

2012-02-01

Full Text Available The removal of mercury from flue gases in scrubbers is greatly facilitated if the mercury is present as water-soluble oxidized species. Therefore, increased mercury oxidation upstream of scrubber devices will improve overall mercury removal. For this purpose heterogeneous catalysts have recently attracted a great deal of interest. Selective catalytic reduction (SCR, noble metal and transition metal oxide based catalysts have been investigated at both the laboratory and plant scale with this objective. A review article published in 2006 covers the progress in the elemental mercury (Hgel catalytic oxidation area. This paper brings the review in this area up to date. To this end, 110 papers including several reports and patents are reviewed. For each type of catalyst the possible mechanisms as well as the effect of flue gas components on activity and stability are examined. Advantages and main problems are analyzed. The possible future directions of catalyst development in this environmental research area are outlined.

Highly Dispersed Pseudo-Homogeneous and Heterogeneous Catalysts Synthesized via Inverse Micelle Solutions for the Liquefaction of Coal

Energy Technology Data Exchange (ETDEWEB)

Hampden-Smith, M.; Kawola, J.S.; Martino, A.; Sault, A.G.; Yamanaka, S.A.

1999-01-05

The mission of this project was to use inverse micelle solutions to synthesize nanometer sized metal particles and test the particles as catalysts in the liquefaction of coal and other related reactions. The initial focus of the project was the synthesis of iron based materials in pseudo-homogeneous form. The frost three chapters discuss the synthesis, characterization, and catalyst testing in coal liquefaction and model coal liquefaction reactions of iron based pseudo-homogeneous materials. Later, we became interested in highly dispersed catalysts for coprocessing of coal and plastic waste. Bifunctional catalysts . to hydrogenate the coal and depolymerize the plastic waste are ideal. We began studying, based on our previously devised synthesis strategies, the synthesis of heterogeneous catalysts with a bifunctional nature. In chapter 4, we discuss the fundamental principles in heterogeneous catalysis synthesis with inverse micelle solutions. In chapter 5, we extend the synthesis of chapter 4 to practical systems and use the materials in catalyst testing. Finally in chapter 6, we return to iron and coal liquefaction now studied with the heterogeneous catalysts.

Nanoporous PdCo Catalyst for Microfuel Cells: Electrodeposition and Dealloying

Directory of Open Access Journals (Sweden)

Satoshi Tominaka

2011-01-01

Full Text Available PdCo alloy is a promising catalyst for oxygen reduction reaction of direct methanol fuel cells because of its high activity and the tolerance to methanol. We have applied this catalyst in order to realize on-chip fuel cell which is a membraneless design. The novel design made the fuel cells to be flexible and integratable with other microdevices. Here, we summarize our recent research on the synthesis of nanostructured PdCo catalyst by electrochemical methods, which enable us to deposit the alloy onto microelectrodes of the on-chip fuel cells. First, the electrodeposition of PdCo is discussed in detail, and then, dealloying for introducing nanopores into the electrodeposits is described. Finally, electrochemical response and activities are fully discussed.

Substrate-Directed Catalytic Selective Chemical Reactions.

Science.gov (United States)

Sawano, Takahiro; Yamamoto, Hisashi

2018-05-04

The development of highly efficient reactions at only the desired position is one of the most important subjects in organic chemistry. Most of the reactions in current organic chemistry are reagent- or catalyst-controlled reactions, and the regio- and stereoselectivity of the reactions are determined by the inherent nature of the reagent or catalyst. In sharp contrast, substrate-directed reaction determines the selectivity of the reactions by the functional group on the substrate and can strictly distinguish sterically and electronically similar multiple reaction sites in the substrate. In this Perspective, three topics of substrate-directed reaction are mainly reviewed: (1) directing group-assisted epoxidation of alkenes, (2) ring-opening reactions of epoxides by various nucleophiles, and (3) catalytic peptide synthesis. Our newly developed synthetic methods with new ligands including hydroxamic acid derived ligands realized not only highly efficient reactions but also pinpointed reactions at the expected position, demonstrating the substrate-directed reaction as a powerful method to achieve the desired regio- and stereoselective functionalization of molecules from different viewpoints of reagent- or catalyst-controlled reactions.

Method of treating emissions of a hybrid vehicle with a hydrocarbon absorber and a catalyst bypass system

Science.gov (United States)

Roos, Bryan Nathaniel; Gonze, Eugene V; Santoso, Halim G; Spohn, Brian L

2014-01-14

A method of treating emissions from an internal combustion engine of a hybrid vehicle includes directing a flow of air created by the internal combustion engine when the internal combustion engine is spinning but not being fueled through a hydrocarbon absorber to collect hydrocarbons within the flow of air. When the hydrocarbon absorber is full and unable to collect additional hydrocarbons, the flow of air is directed through an electrically heated catalyst to treat the flow of air and remove the hydrocarbons. When the hydrocarbon absorber is not full and able to collect additional hydrocarbons, the flow of air is directed through a bypass path that bypasses the electrically heated catalyst to conserve the thermal energy stored within the electrically heated catalyst.

Production of Biodiesel from Shea Butter Oil using Homogeneous Catalysts

Directory of Open Access Journals (Sweden)

Jude EJEH

2014-02-01

Full Text Available An investigation into the production of biodiesel from shea butter oil using homogenous catalyst was carried out. The properties of the oil obtained were first determined, having an FFA value of 2.279 amongst other properties. Thus, the direct base-catalysis method was used, with potassium hydroxide as the catalyst. In a 1 hour batch run, biodiesel was produced with a conversion of 92%, FAME content of 97.1%, cetane number of 46.84 and kinematic viscosity of 4.30mm2/s, conforming to ASTM D6751 and EN 14214 international standards. As such, it was established that shea butter biodiesel could be produced by the direct base catalysis, over a shorter time with low cost chemicals.

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....

Non-PGM cell catalysts

Energy Technology Data Exchange (ETDEWEB)

Colon-Mercado, H. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Elvington, M. [Savannah River Consulting, Aiken, SC (United States); Ganesan, P. [Savannah River Consulting, Aiken, SC (United States)

2017-09-27

A unique approach has been developed to probe the non-PGM catalyst active site for the Oxygen Reduction Reaction (ORR) for PEMFCs. Iron based functionalities have been engineered into a variety of catalysts to evaluate their impact on activity for the ORR. A series of high surface area catalysts were synthesized and the impact of the chemical structure on the electrochemical and electrocatalytic properties was investigated. Elemental and surface analyses of the prepared catalysts reveal the incorporation of iron in a targeted and controlled manner. A high surface area framework catalyst was prepared that shows exceptional activity, comparable to state-of-the-art materials. The results of this research project provided critical seed data for the newly awarded ElectroCat project, which focuses on rationally designed framework catalysts for the oxygen reduction reaction.

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.

Iron(II) phthalocyanine covalently functionalized graphene as a highly efficient non-precious-metal catalyst for the oxygen reduction reaction in alkaline media

International Nuclear Information System (INIS)

Liu, Ying; Wu, Yan-Ying; Lv, Guo-Jun; Pu, Tao; He, Xing-Quan; Cui, Li-Li

2013-01-01

Graphical abstract: The fabricated FePc-Gr catalyst for ORR exhibited high activity, favoring a direct 4-electron process, good stability and selectivity, all of which should be attributed to its high conductivity, the synergistic effect between FePc and graphene, as well as the formation of stable FePc-Gr composite through covalent bonding and π–π interaction. - Abstract: A novel iron(II) phthalocyanine covalently modified graphene (FePc-Gr) was synthesized by reduction of the product obtained through an amidation reaction between carboxyl-functionalized graphene oxide (CFGO) and iron(II) tetra-aminophthalocyanine (FeTAPc). The FePc-Gr hybird was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectroscopy (RS) and X-ray photoelectron spectroscopy (XPS), respectively. The electrocatalytic properties of FePc-Gr toward the oxygen reduction reaction (ORR) were evaluated using cyclic voltammetry (CV) and linear sweep voltammetry methods. The peak potential of the ORR on the FePc-Gr catalyst was found to be about −0.12 V vs. SCE in 0.1 M NaOH solution, which was 180 and 360 mV more positive than that on FeTAPc and bare GCE, respectively. The rotating disk electrode (RDE) and rotating ring disk electrode (RRDE) measurements revealed that the ORR mechanism was nearly via a direct four-electron pathway to water on FePc-Gr. The current still remained 83.5% of its initial after chronoamperometric test for 10,000 s. Nevertheless, Pt/C catalyst only retained 40.5% of its initial current. The peak potential and peak current changed slightly when 3 M methanol was introduced. So the FePc-Gr composite catalyst for ORR exhibited high activity, good stability and methanol-tolerance, which could be used as a promising Pt-free catalyst for ORR in alkaline direct methanol fuel cell (DMFC)

Alloy catalyst material

DEFF Research Database (Denmark)

2014-01-01

The present invention relates to a novel alloy catalyst material for use in the synthesis of hydrogen peroxide from oxygen and hydrogen, or from oxygen and water. The present invention also relates to a cathode and an electrochemical cell comprising the novel catalyst material, and the process use...... of the novel catalyst material for synthesising hydrogen peroxide from oxygen and hydrogen, or from oxygen and water....

The black rock series supported SCR catalyst for NO x removal.

Science.gov (United States)

Xie, Bin; Luo, Hang; Tang, Qing; Du, Jun; Liu, Zuohua; Tao, Changyuan

2017-09-01

Black rock series (BRS) is of great potential for their plenty of valued oxides which include vanadium, iron, alumina and silica oxides, etc. BRS was used for directly preparing of selective catalytic reduction (SCR) catalyst by modifying its surface texture with SiO 2 -TiO 2 sols and regulating its catalytic active constituents with V 2 O 5 and MoO 3 . Consequently, 90% NO removal ratio was obtained within 300-400 °C over the BRS-based catalyst. The structure and properties of the BRS-based catalyst were characterized by the techniques of N 2 adsorption-desorption, X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), H 2 -temperature programmed reduction (H 2 -TPR), and NH 3 -temperature programmed desorption (NH 3 -TPD). The results revealed that the BRS-based catalyst possesses favorable properties for NO x removal, including highly dispersed active components, abundant surface-adsorbed oxygen O α , well redox property, and numerous Brønsted acid sites. Particularly, the BRS-based catalyst exhibited considerable anti-poisoning performance compared with commercial TiO 2 -based catalyst. The former catalyst shows a NO conversion surpassing 80% from 300 to 400 °C for potassium poisoning, and a durability of SO 2 and H 2 O exceeding 85% at temperatures from 300 to 450 °C.

Potassium effects on kinetics of propane oxydehydrogenation on vanadia-titania catalyst

International Nuclear Information System (INIS)

Grabowski, R.; Samson, K.

2003-01-01

Oxidative dehydrogenation of propane (ODH) over V 2 O 5 /TiO 2 and V 2 O 5 /TiO 2 doped with K was carried out by measuring conversions and selectiveness for various feed compositions, contact times and temperatures. The results obtained for both catalysts were interpreted on the basis of the mechanism, in which propene is formed through Eley-Rideal sequence of steps, i.e. without participation of the adsorbed propane species. Kinetic constants (activation energies, pre-exponential factors) for the model of ODH reaction of propane on these catalysts, obtained on the basis of steady-state results, are given. Addition of K to vanadia-titania catalysts leads to decrease of total combustion of propane and consecutive combustion of propene. It has been found that the direct propane total oxidation is 5 - 9 times lower than that of the consecutive propene oxidation and is almost temperature independent for potassium doped catalyst, whereas it quickly decreases with temperature for a non-doped catalyst. Secondly, the addition of K to a vanadia-titania catalyst decreases the activation energies for propene formation (k 1 ), parallel formation of CO x (k 3 ) and reoxidation of the catalyst (k os ). Potassium exhibits a stronger inhibitory effect on the secondary propene combustion, what reflects the lower activity of V 5+ cations modified by the strongly basic alkali oxide species. (author)

Combinatorial discovery of new methanol-tolerant non-noble metal cathode electrocatalysts for direct methanol fuel cells.

Science.gov (United States)

Yu, Jong-Sung; Kim, Min-Sik; Kim, Jung Ho

2010-12-14

Combinatorial synthesis and screening were used to identify methanol-tolerant non-platinum cathode electrocatalysts for use in direct methanol fuel cells (DMFCs). Oxygen reduction consumes protons at the surface of DMFC cathode catalysts. In combinatorial screening, this pH change allows one to differentiate active catalysts using fluorescent acid-base indicators. Combinatorial libraries of carbon-supported catalyst compositions containing Ru, Mo, W, Sn, and Se were screened. Ternary and quaternary compositions containing Ru, Sn, Mo, Se were more active than the "standard" Alonso-Vante catalyst, Ru(3)Mo(0.08)Se(2), when tested in liquid-feed DMFCs. Physical characterization of the most active catalysts by powder X-ray diffraction, gas adsorption, and X-ray photoelectron spectroscopy revealed that the predominant crystalline phase was hexagonal close-packed (hcp) ruthenium, and showed a surface mostly covered with oxide. The best new catalyst, Ru(7.0)Sn(1.0)Se(1.0), was significantly more active than Ru(3)Se(2)Mo(0.08), even though the latter contained smaller particles.

Performance characterization of hydrogen isotope exchange and recombination catalysts for tritium processing

International Nuclear Information System (INIS)

Suppiah, S.; Ryland, D.; Marcinkowska, K.; Boniface, H.; Everatt, A.

2010-01-01

AECL's hydrogen isotope exchange catalyst and recombination catalysts have been successfully applied to a wide range of industrial tritium-removal applications. The catalysts are used for Liquid Phase Catalytic Exchange (LPCE) and for gas-phase and trickle-bed recombination of hydrogen isotopes and have led to process simplification, improved safety and operational advantages. Catalyst performance design equations derived from laboratory testing of these catalysts have been validated against performance under industrial conditions. In a Combined Electrolysis and Catalytic Exchange (CECE) demonstration plant analyses of LPCE and recombiner efficiency were carried out as a function of catalyst activity over a wide range of operation. A steady-state process simulation used to model and design the hydrogen-water isotopic exchange processes, such as the CECE detritiation plant, was validated using the results of this demonstration. Catalyst development for isotope-exchange and recombination applications has continued over the last decade. As a result, significant improvements in catalyst performance have been achieved for these applications. This paper outlines the uniqueness of AECL's specialized catalysts and process designs for these applications with examples from laboratory and industrial case studies.

Biomass Conversion over Heteropoly Acid Catalysts

KAUST Repository

Zhang, Jizhe

2015-04-01

(Au/Cs2HPW12O40) that enabled the selective conversion of cellobiose to gluconic acid with a very high yield of 96.4% (Chapter II); we realized a direct oxidative conversion of cellulose to glycolic acid (yield of 49.3 %) in a water medium for the first time, by using a phosphomolybdic acid catalyst (chapter III); we found that a vanadium-substituted phosphomolybdic acid catalyst (H4PVMo11O40) is capable of converting various biomass-derived substrates to formic acid and acetic acid with high selectivity, and under optimized reaction conditions, high yield of formic acid (67.8%) can be obtained from cellulose (chapter IV); we discovered that the vanadium-substituted phosphomolybdic acids can also selectively oxidize glycerol, a low-cost by-product of biodiesel, to formic acid, and interestingly this conversion can be performed in highly concentration aqueous solution (glycerol: water = 50: 50), giving rise to exceptionally high conversion efficiency (chapter V). These results reveal that HPAs are useful and suitable catalysts for selective oxidation of biomass, and that the reaction pathway is largely determined by the type of addenda atom in the HPA catalyst. The optimization of the reaction conditions and processes in these systems are also discussed in this thesis.

Introducing catalyst in alkaline membrane for improved performance direct borohydride fuel cells

Science.gov (United States)

Qin, Haiying; Lin, Longxia; Chu, Wen; Jiang, Wei; He, Yan; Shi, Qiao; Deng, Yonghong; Ji, Zhenguo; Liu, Jiabin; Tao, Shanwen

2018-01-01

A catalytic material is introduced into the polymer matrix to prepare a novel polymeric alkaline electrolyte membrane (AEM) which simultaneously increases ionic conductivity, reduces the fuel cross-over. In this work, the hydroxide anion exchange membrane is mainly composed of poly(vinylalcohol) and alkaline exchange resin. CoCl2 is added into the poly(vinylalcohol) and alkaline exchange resin gel before casting the membrane to introduce catalytic materials. CoCl2 is converted into CoOOH after the reaction with KOH solution. The crystallinity of the polymer matrix decreases and the ionic conductivity of the composite membrane is notably improved by the introduction of Co-species. A direct borohydride fuel cell using the composite membrane exhibits an open circuit voltage of 1.11 V at 30 °C, which is notably higher than that of cells using other AEMs. The cell using the composite membrane achieves a maximum power density of 283 mW cm-2 at 60 °C while the cell using the membrane without Co-species only reaches 117 mW cm-2 at the same conditions. The outstanding performance of the cell using the composite membrane benefits from impregnation of the catalytic Co-species in the membrane, which not only increases the ionic conductivity but also reduces electrode polarization thus improves the fuel cell performance. This work provides a new approach to develop high-performance fuel cells through adding catalysts in the electrolyte membrane.

Coatings of active and heat-resistant cobalt-aluminium xerogel catalysts.

Science.gov (United States)

Schubert, Miriam; Schubert, Lennart; Thomé, Andreas; Kiewidt, Lars; Rosebrock, Christopher; Thöming, Jorg; Roessner, Frank; Bäumer, Marcus

2016-09-01

The application of catalytically coated metallic foams in catalytic processes has a high potential for exothermic catalytic reactions such as CO2 methanation or Fischer-Tropsch synthesis due to good heat conductivity, improved turbulent flow properties and high catalyst efficiencies. But the preparation of homogenous catalyst coats without pore blocking is challenging with conventional wash coating techniques. Here, we report on a stable and additive free colloidal CoAlOOH suspension (sol) for the preparation of catalytically active Co/Al2O3 xerogel catalysts and coatings. Powders with 18wt% Co3O4 prepared from this additive free synthesis route show a catalytic activity in Fischer-Tropsch synthesis and CO2 methanation which is similar to a catalyst prepared by incipient wetness impregnation (IWI) after activating the material under flowing hydrogen at 430°C. Yet, the xerogel catalyst exhibits a much higher thermal stability as compared to the IWI catalyst, as demonstrated in catalytic tests after different heat agings between 430°C and 580°C. It was also found that the addition of polyethylene glycol (PEG) to the sol influences the catalytic properties of the formed xerogels negatively. Only non-reducible cobalt spinels were formed from a CoAlOOH sol with 20wt% PEG. Metallic foams with pores sizes between 450 and 1200μm were coated with the additive free CoAlOOH sol, which resulted in homogenous xerogel layers. First catalytic tests of the coated metal foams (1200μm) showed good performance in CO2 methanation. Copyright © 2016 Elsevier Inc. All rights reserved.

Catalyst for microelectromechanical systems microreactors

Science.gov (United States)

Morse, Jeffrey D [Martinez, CA; Sopchak, David A [Livermore, CA; Upadhye, Ravindra S [Pleasanton, CA; Reynolds, John G [San Ramon, CA; Satcher, Joseph H [Patterson, CA; Gash, Alex E [Brentwood, CA

2010-06-29

A microreactor comprising a silicon wafer, a multiplicity of microchannels in the silicon wafer, and a catalyst coating the microchannels. In one embodiment the catalyst coating the microchannels comprises a nanostructured material. In another embodiment the catalyst coating the microchannels comprises an aerogel. In another embodiment the catalyst coating the microchannels comprises a solgel. In another embodiment the catalyst coating the microchannels comprises carbon nanotubes.

Fibrous Catalyst-Enhanced Acanthamoeba Disinfection by Hydrogen Peroxide.

Science.gov (United States)

Kilvington, Simon; Winterton, Lynn

2017-11-01

Hydrogen peroxide (H2O2) disinfection systems are contact-lens-patient problem solvers. The current one-step, criterion-standard version has been widely used since the mid-1980s, without any significant improvement. This work identifies a potential next-generation, one-step H2O2, not based on the solution formulation but rather on a case-based peroxide catalyst. One-step H2O2 systems are widely used for contact lens disinfection. However, antimicrobial efficacy can be limited because of the rapid neutralization of the peroxide from the catalytic component of the systems. We studied whether the addition of an iron-containing catalyst bound to a nonfunctional propylene:polyacryonitrile fabric matrix could enhance the antimicrobial efficacy of these one-step H2O2 systems. Bausch + Lomb PeroxiClear and AOSept Plus (both based on 3% H2O2 with a platinum-neutralizing disc) were the test systems. These were tested with and without the presence of the catalyst fabric using Acanthamoeba cysts as the challenge organism. After 6 hours' disinfection, the number of viable cysts was determined. In other studies, the experiments were also conducted with biofilm formed by Stenotrophomonas maltophilia and Elizabethkingia meningoseptica bacteria. Both control systems gave approximately 1-log10 kill of Acanthamoeba cysts compared with 3.0-log10 kill in the presence of the catalyst (P catalyst compared with ≥3.0-log10 kill when it was omitted. In 30 rounds' recurrent usage, the experiments, in which the AOSept Plus system was subjected to 30 rounds of H2O2 neutralization with or without the presence of catalytic fabric, showed no loss in enhanced biocidal efficacy of the material. The catalytic fabric was also shown to not retard or increase the rate of H2O2 neutralization. We have demonstrated the catalyst significantly increases the efficacy of one-step H2O2 disinfection systems using highly resistant Acanthamoeba cysts and bacterial biofilm. Incorporating the catalyst into the

In situ, Cr K-edge XAS study on the Phillips catalyst : activation and ethylene polymerization

NARCIS (Netherlands)

Groppo, E.; Prestipino, C.; Cesano, F.; Bonino, F.; Bordiga, S.; Lamberti, C.; Thuene, P.C.; Niemantsverdriet, J.W.; Zecchina, A.

2005-01-01

In this in situ EXAFS and XANES study on the Phillips ethylene-polymerization Cr/SiO2 catalyst, two polymerization routes are investigated and compared. The first mimics that adopted in industrial plants, where ethylene is dosed directly on the oxidized catalyst, while in the second the oxidized

Surface noble metal modified PdM/C (M = Ru, Pt, Au) as anode catalysts for direct ethanol fuel cells

International Nuclear Information System (INIS)

Mao, Han; Huang, Tao; Yu, Aishui

2016-01-01

In this article, we studied the surface noble metal modification on Pd nanoparticles, other than the homogeneous or core-shell structure. The surface modification will lead to the uneven constitution within the nanoparticles and thus more obvious optimization effect toward the catalyst brought by the lattice deformation. The surface of the as-prepared Pd nanoparticles was modified with Ru, Pt or Au by a moderate and green approach, respectively. XPS results confirm the interactive electron effects between Pd and the modified noble metal. Electrochemical measurements show that the surface noble metal modified catalysts not only show higher catalytic activity, but also better stability and durability. The PdM/C catalysts all exhibit good dispersion and very little agglomeration after long-term potential cycles toward ethanol oxidation. With only 10% metallic atomic ratio of Au, PdAu/C catalyst shows extraordinary catalytic activity and stability, the peak current reaches 1700 mA mg"−"1 Pd, about 2.5 times that of Pd/C. Moreover, the PdAu/C maintains 40% of the catalytic activity after 4500 potential cycles. - Highlights: • Pd-based catalysts with complicated exposed facets. • Much enhanced electrocatalytic activity and stability with about 10% noble metal M (M = Ru, Pt, Au) on Pd nanoparticles. • The outstanding electrocatalytic performance of PdAu/C towards ethanol oxidation after the Au modification.

Surface noble metal modified PdM/C (M = Ru, Pt, Au) as anode catalysts for direct ethanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Mao, Han; Huang, Tao, E-mail: huangt@fudan.edu.cn; Yu, Aishui, E-mail: asyu@fudan.edu.cn

2016-08-15

In this article, we studied the surface noble metal modification on Pd nanoparticles, other than the homogeneous or core-shell structure. The surface modification will lead to the uneven constitution within the nanoparticles and thus more obvious optimization effect toward the catalyst brought by the lattice deformation. The surface of the as-prepared Pd nanoparticles was modified with Ru, Pt or Au by a moderate and green approach, respectively. XPS results confirm the interactive electron effects between Pd and the modified noble metal. Electrochemical measurements show that the surface noble metal modified catalysts not only show higher catalytic activity, but also better stability and durability. The PdM/C catalysts all exhibit good dispersion and very little agglomeration after long-term potential cycles toward ethanol oxidation. With only 10% metallic atomic ratio of Au, PdAu/C catalyst shows extraordinary catalytic activity and stability, the peak current reaches 1700 mA mg{sup −1} Pd, about 2.5 times that of Pd/C. Moreover, the PdAu/C maintains 40% of the catalytic activity after 4500 potential cycles. - Highlights: • Pd-based catalysts with complicated exposed facets. • Much enhanced electrocatalytic activity and stability with about 10% noble metal M (M = Ru, Pt, Au) on Pd nanoparticles. • The outstanding electrocatalytic performance of PdAu/C towards ethanol oxidation after the Au modification.

Optimization of Rhodium-Based Catalysts for Mixed Alcohol Synthesis – 2012 Progress Report

Energy Technology Data Exchange (ETDEWEB)

Gerber, Mark A.; Gray, Michel J.; Albrecht, Karl O.; Thompson, Becky L.

2012-11-01

Pacific Northwest National Laboratory has been conducting research to investigate the feasibility of producing mixed alcohols from biomass-derived synthesis gas (syngas). In recent years, this research has primarily involved the further development of catalysts containing rhodium and manganese based on the results of earlier catalyst screening tests. Testing continued in FY 2012 to further improve the Ir-promoted RhMn catalysts on both silica and carbon supports for producing mixed oxygenates from synthesis gas. This testing re-examined selected alternative silica and carbon supports to follow up on some uncertainties in the results with previous test results. Additional tests were conducted to further optimize the total and relative concentrations of Rh, Mn, and Ir, and to examine selected promoters and promoter combinations based on earlier results. To establish optimum operating conditions, the effects of the process pressure and the feed gas composition also were evaluated.

DEVELOPMENT OF ATTRITION RESISTANT IRON-BASED FISCHER-TROPSCH CATALYSTS

International Nuclear Information System (INIS)

Adeyinka A. Adeyiga

2001-01-01

The Fischer-Tropsch (F-T) reaction provides a way of converting coal-derived synthesis gas (CO+H 2 ) to liquid fuels. Since the reaction is highly exothermic, one of the major problems in control of the reaction is heat removal. Recent work has shown that the use of slurry bubble column reactors (SBCRs) can largely solve this problem. The use of iron-based catalysts is attractive not only due to their low cost and ready availability, but also due to their high water-gas shift activity which makes it possible to use these catalysts with low H 2 /CO ratios. However, a serious problem with use of Fe catalysts in a SBCR is their tendency to undergo attrition. This can cause fouling/plugging of downstream filters and equipment, makes the separation of catalyst from the oil/wax product very difficult if not impossible, and results in a steady loss of catalyst from the reactor. Recently, fundamental understanding of physical attrition is being addressed by incorporating suitable binders into the catalyst recipe. This has resulted in the preparation of a spray dried Fe-based catalyst having aps of 70 mm with high attrition resistance. This Fe-based attrition resistant, active and selective catalyst gave 95% CO conversion through 125 hours of testing in a fixed-bed at 270 C, 1.48 MPa, H 2 /CO=0.67 and 2.0 NL/g-cat/h with C 5 + selectivity of >78% and methane selectivity of <5%. However, further development of the catalyst is needed to address the chemical attrition due to phase changes that any Fe-catalyst goes through potentially causing internal stresses within the particle and resulting in weakening, spalling or cracking. The objective of this research is to develop robust iron-based Fischer-Tropsch catalysts that have suitable activity, selectivity and stability to be used in the slurry bubble column reactor. Specifically we aim to develop to: (i) improve the performance and preparation procedure of the high activity, high attrition resistant, high alpha iron