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Sample records for efficient pt catalysts

  1. Pt and PtRu catalyst bilayers increase efficiencies for ethanol oxidation in proton exchange membrane electrolysis and fuel cells

    Science.gov (United States)

    Altarawneh, Rakan M.; Pickup, Peter G.

    2017-10-01

    Polarization curves, product distributions, and reaction stoichiometries have been measured for the oxidation of ethanol at anodes consisting of Pt and PtRu bilayers and a homogeneous mixture of the two catalysts. These anode structures all show synergies between the two catalysts that can be attributed to the oxidation of acetaldehyde produced at the PtRu catalyst by the Pt catalyst. The use of a PtRu layer over a Pt layer produces the strongest effect, with higher currents than a Pt on PtRu bilayer, mixed layer, or either catalyst alone, except for Pt at high potentials. Reaction stoichiometries (average number of electrons transferred per ethanol molecule) were closer to the values for Pt alone for both of the bilayer configurations but much lower for PtRu and mixed anodes. Although Pt alone would provide the highest overall fuel cell efficiency at low power densities, the PtRu on Pt bilayer would provide higher power densities without a significant loss of efficiency. The origin of the synergy between the Pt and PtRu catalysts was elucidated by separation of the total current into the individual components for generation of carbon dioxide and the acetaldehyde and acetic acid byproducts.

  2. Bimetallic Ag-Pt Sub-nanometer Supported Clusters as Highly Efficient and Robust Oxidation Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Negreiros, Fabio R. [CNR-ICCOM & IPCF, Consiglio Nazionale delle Ricerche, Pisa Italy; Halder, Avik [Materials Science Division, Argonne National Laboratory, Lemont IL USA; Yin, Chunrong [Materials Science Division, Argonne National Laboratory, Lemont IL USA; Singh, Akansha [Harish-Chandra Research Institute, HBNI, Chhatnag Road Jhunsi Allahabad 211019 India; Barcaro, Giovanni [CNR-ICCOM & IPCF, Consiglio Nazionale delle Ricerche, Pisa Italy; Sementa, Luca [CNR-ICCOM & IPCF, Consiglio Nazionale delle Ricerche, Pisa Italy; Tyo, Eric C. [Materials Science Division, Argonne National Laboratory, Lemont IL USA; Pellin, Michael J. [Materials Science Division, Argonne National Laboratory, Lemont IL USA; Bartling, Stephan [Institut für Physik, Universität Rostock, Rostock Germany; Meiwes-Broer, Karl-Heinz [Institut für Physik, Universität Rostock, Rostock Germany; Seifert, Sönke [X-ray Science Division, Argonne National Laboratory, Lemont IL USA; Sen, Prasenjit [Harish-Chandra Research Institute, HBNI, Chhatnag Road Jhunsi Allahabad 211019 India; Nigam, Sandeep [Chemistry Division, Bhabha Atomic Research Centre, Trombay Mumbai- 400 085 India; Majumder, Chiranjib [Chemistry Division, Bhabha Atomic Research Centre, Trombay Mumbai- 400 085 India; Fukui, Nobuyuki [East Tokyo Laboratory, Genesis Research Institute, Inc., Ichikawa Chiba 272-0001 Japan; Yasumatsu, Hisato [Cluster Research Laboratory, Toyota Technological Institute: in, East Tokyo Laboratory, Genesis Research Institute, Inc. Ichikawa, Chiba 272-0001 Japan; Vajda, Stefan [Materials Science Division, Argonne National Laboratory, Lemont IL USA; Nanoscience and Technology Division, Argonne National Laboratory, Lemont IL USA; Institute for Molecular Engineering, University of Chicago, Chicago IL USA; Fortunelli, Alessandro [CNR-ICCOM & IPCF, Consiglio Nazionale delle Ricerche, Pisa Italy; Materials and Process Simulation Center, California Institute of Technology, Pasadena CA USA

    2017-12-29

    A combined experimental and theoretical investigation of Ag-Pt sub-nanometer clusters as heterogeneous catalysts in the CO -> CO2 reaction (COox) is presented. Ag9Pt2 and Ag9Pt3 clusters are size-selected in the gas phase, deposited on an ultrathin amorphous alumina support, and tested as catalysts experimentally under realistic conditions and by first-principles simulations at realistic coverage. Insitu GISAXS/TPRx demonstrates that the clusters do not sinter or deactivate even after prolonged exposure to reactants at high temperature, and present comparable, extremely high COox catalytic efficiency. Such high activity and stability are ascribed to a synergic role of Ag and Pt in ultranano-aggregates, in which Pt anchors the clusters to the support and binds and activates two CO molecules, while Ag binds and activates O-2, and Ag/Pt surface proximity disfavors poisoning by CO or oxidized species.

  3. Pt-based Thin Films as Efficient and Stable Catalysts for Oxygen Electroreduction

    DEFF Research Database (Denmark)

    Zamburlini, Eleonora

    at the cathode of Polymer Electrolyte Membrane Fuel Cells (PEMFCs). Herein the fabrication method, which consists of co-sputtering of thin films, is presented in detail, explaining the challenges one must face in order to fabricate oxygen-free Pt-lanthanides and Pt-early transition metals alloys......This thesis presents the fabrication and characterization of Pt-based thin film catalysts for Oxygen Reduction Reaction (ORR). Gadolinium and Yttrium have been used as alloying materials, in preparation for the replacement of the traditional but economically disadvantageous pure Pt catalysts......, and the proposed solutions. The characterization of the catalysts focused mainly on the electrochemical testing using a Rotating Ring Disk Electrode (RRDE) setup, and includes X-ray Diffraction (XRD), X-ray Photoemission Spectroscopy (XPS), Angle-Resolved X-ray Photoelectron Spectroscopy (AR-XPS), Scanning...

  4. Efficient hydrodeoxygenation of biomass-derived ketones over bifunctional Pt-polyoxometalate catalyst.

    Science.gov (United States)

    Alotaibi, Mshari A; Kozhevnikova, Elena F; Kozhevnikov, Ivan V

    2012-07-21

    Acidic heteropoly salt Cs(2.5)H(0.5)PW(12)O(40) doped with Pt nanoparticles is a highly active and selective catalyst for one-step hydrogenation of methyl isobutyl and diisobutyl ketones to the corresponding alkanes in the gas phase at 100 °C with 97-99% yield via metal-acid bifunctional catalysis.

  5. Bimetallic magnetic PtPd-nanoparticles as efficient catalyst for PAH removal from liquid media

    Science.gov (United States)

    Zanato, A. F. S.; Silva, V. C.; Lima, D. A.; Jacinto, M. J.

    2017-11-01

    Monometallic Pd- and bimetallic PtPd-nanoparticles supported on a mesoporous magnetic magnetite@silica matrix resembling a core-shell structure (Fe3O4@mSiO2) have been fabricated. The material was characterized by transmission electron microscope (TEM), high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectra (XPS), energy dispersive spectroscopy (EDS) and inductively coupled plasma mass spectrometry (ICP-MS). The catalysts were applied in the removal of anthracene from liquid phase via catalytic hydrogenation. It was found that anthracene as a model compound could be completely converted into the partially hydrogenated species by the monometallic and bimetallic solids. However, during the recycling study the bimetallic material (Fe3O4@mSiO2PtPd-) showed an enhanced activity towards anthracene removal compared with the monometallic materials. A single portion of the PtPd-based catalyst can be used up to 11 times in the hydrogenation of anthracene under mild conditions (6 atm of H2, 75 °C, 20 min). Thanks to the presence of a dense magnetic core, the catalysts were capable of responding to an applied external magnetic field and once the reaction was completed, catalyst/product separation was straightforward.

  6. Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C-H activation

    Science.gov (United States)

    Marcinkowski, Matthew D.; Darby, Matthew T.; Liu, Jilei; Wimble, Joshua M.; Lucci, Felicia R.; Lee, Sungsik; Michaelides, Angelos; Flytzani-Stephanopoulos, Maria; Stamatakis, Michail; Sykes, E. Charles H.

    2018-03-01

    The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards the synthesis of fuels and fine chemicals. Heterogeneous catalysts based on Ni and Pt can perform this chemistry, but deactivate easily due to coke formation. Cu-based catalysts are not practical due to high C-H activation barriers, but their weaker binding to adsorbates offers resilience to coking. Using Pt/Cu single-atom alloys (SAAs), we examine C-H activation in a number of systems including methyl groups, methane and butane using a combination of simulations, surface science and catalysis studies. We find that Pt/Cu SAAs activate C-H bonds more efficiently than Cu, are stable for days under realistic operating conditions, and avoid the problem of coking typically encountered with Pt. Pt/Cu SAAs therefore offer a new approach to coke-resistant C-H activation chemistry, with the added economic benefit that the precious metal is diluted at the atomic limit.

  7. Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation

    Energy Technology Data Exchange (ETDEWEB)

    Marcinkowski, Matthew D.; Darby, Matthew T.; Liu, Jilei; Wimble, Joshua M.; Lucci, Felicia R.; Lee, Sungsik; Michaelides, Angelos; Flytzani-Stephanopoulos, Maria; Stamatakis, Michail; Sykes, E. Charles H.

    2018-01-08

    The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards synthesis of fuels and fine chemicals. Heterogeneous catalysts based on Ni and Pt can perform this chemistry, but deactivate easily due to coke formation. Cu- based catalysts are not practical for this chemistry due to high C-H activation barriers, but their weaker binding to adsorbates offers resilience to coking. Utilizing Pt/Cu single atom alloys (SAAs) we examine C-H activation in a number of systems including methyl groups, methane, and butane using a combination of simulations, surface science, and catalysis studies. We find that Pt/Cu SAAs activate C-H bonds more efficiently than Cu, are stable for days under realistic operating conditions, and avoid the problem of coking typically encountered with Pt. Pt/Cu SAAs therefore offer a new approach to coke resistant C-H activation chemistry with the added economic benefit that the precious metal is diluted at the atomic limit.

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

    Science.gov (United States)

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

    2018-06-04

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

  9. Radiolytic Synthesis of Pt-Ru Catalysts Based on Functional Polymer-Grafted MWNT and Their Catalytic Efficiency for CO and MeOH

    Directory of Open Access Journals (Sweden)

    Dae-Soo Yang

    2011-01-01

    Full Text Available Pt-Ru catalysts based on functional polymer-grafted MWNT (Pt-Ru@FP-MWNT were prepared by radiolytic deposition of Pt-Ru nanoparticles on functional polymer-grafted multiwalled carbon nanotube (FP-MWNT. Three different types of functional polymers, poly(acrylic acid (PAAc, poly(methacrylic acid (PMAc, and poly(vinylphenyl boronic acid (PVPBAc, were grafted on the MWNT surface by radiation-induced graft polymerization (RIGP. Then, Pt-Ru nanoparticles were deposited onto the FP-MWNT supports by the reduction of metal ions using γ-irradiation to obtain Pt-Ru@FP-MWNT catalysts. The Pt-Ru@FP-MWNT catalysts were then characterized by XRD, XPS, TEM ,and elemental analysis. The catalytic efficiency of Pt-Ru@FP-MWNT catalyst was examined for CO stripping and MeOH oxidation for use in a direct methanol fuel cell (DMFC. The Pt-Ru@PVPBAc-MWNT catalyst shows enhanced activity for electro-oxidation of CO and MeOH oxidation over that of the commercial E-TEK catalyst.

  10. Efficient photocatalytic hydrogen production from water over Pt-Eosin Y catalyst: A systemic study of reaction parameters

    Science.gov (United States)

    Wang, Li; Zhao, Hui; Chen, Yong; Sun, Ruimin; Han, Bing

    2016-07-01

    A high efficient homogeneous system for hydrogen production from water consisting of Eosin Y as a photosensitizer, methyl viologen (MV2+) as an electron transfer mediator, triethanolamine (TEOA) as a sacrificial electron donor and colloid Pt as a catalyst, has been systemicly studied. The initial system pH and the concentration of Eosin Y have remarkable effects on the rate of hydrogen evolution. The optimal pH and concentration of Eosin Y are 9 and 7.2×10-5 M. Triethanolamine (TEOA) as an electron donor, can reductively quench the oxidized Eosin Y and the quenching is well modeled by the Stern-Volmer equation. The optimal concentration of TEOA and the concentration of MV2+ are 0.3 M and 3.1×10-4 M, respectively. In addition, the role of colloid Pt has been investigated.

  11. Properties and efficiency of a Pt/Al2O3 catalyst applied in a solid fuel thermo-accumulating furnace

    Directory of Open Access Journals (Sweden)

    SRDJAN BELOSEVIC

    2007-08-01

    Full Text Available A prototype of a solid fuel thermo-accumulating furnace has been developed. In order to achieve a higher combustion efficiency, a Pt/Al2O3 catalyst in the form of 3 ± 0.3 mm spheres was applied, which enabled further combustion of flue gases within the furnace. Experimental investigation of the influence of the catalyst on the conversion of CO has been done for different operation regimes and positions of the catalyst. Paper presents selected results regarding CO emission during wood and coal combustion. Investigations suggest a considerable effect of the catalyst and a strong influence of the catalyst position to CO emission reduction. The microstructure of the catalyst beads, characterized by selective chemisorption of CO, has shown the decrease of the number of Pt sites as a consequence of blockage by coke deposits formed during the combustion of solid fuel.

  12. 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.

  13. Pt/C Fuel Cell Catalyst Degradation

    DEFF Research Database (Denmark)

    Zana, Alessandro

    This thesis investigates the degradation behavior of Pt/C catalysts under simulated automotive conditions. By using the “tool box” synthesis method the Pt loading has been changed from low to high Pt loadings, therefore permitting to study the role of Pt on the degradation of high surface area (H...

  14. Monodisperse Pt atoms anchored on N-doped graphene as efficient catalysts for CO oxidation: A first-principles investigation

    KAUST Repository

    Liu, Xin; Sui, Yanhui; Duan, Ting; Meng, Changgong; Han, Yu

    2015-01-01

    We performed first-principles based calculations to investigate the electronic structure and the potential catalytic performance of Pt atoms monodispersed on N-doped graphene in CO oxidation. We showed that N-doping can introduce localized defect states in the vicinity of the Fermi level of graphene which will effectively stabilize the deposited Pt atoms. The binding energy of a single Pt atom onto a stable cluster of 3 pyridinic N (PtN3) is up to -4.47 eV, making the diffusion and aggregation of anchored Pt atoms difficult. Both the reaction thermodynamics and kinetics suggest that CO oxidation over PtN3 would proceed through the Langmuir-Hinshelwood mechanism. The reaction barriers for the formation and dissociation of the peroxide-like intermediate are determined to be as low as 0.01 and 0.08 eV, respectively, while that for the regeneration is only 0.15 eV, proving the potential high catalytic performance of PtN3 in CO oxidation, especially at low temperatures. The Pt-d states that are up-shifted by the Pt-N interaction account for the enhanced activation of O2 and the efficient formation and dissociation of the peroxide-like intermediate.

  15. 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

  16. Pt atoms stabilized on hexagonal boron nitride as efficient single-atom catalysts for CO oxidation: A first-principles investigation

    KAUST Repository

    Liu, Xin

    2015-01-01

    Taking CO oxidation as a probe, we investigated the electronic structure and reactivity of Pt atoms stabilized by vacancy defects on hexagonal boron nitride (h-BN) by first-principles-based calculations. As a joint effect of the high reactivity of both a single Pt atom and a boron vacancy defect (PtBV), the Pt-N interaction is -4.40 eV and is already strong enough to prohibit the diffusion and aggregation of the stabilized Pt atom. Facilitated by the upshifted Pt-d states originated from the Pt-N interaction, the barriers for CO oxidation through the Langmuir-Hinshelwood mechanism for formation and dissociation of peroxide-like intermediate and the regeneration are as low as 0.38, 0.10 and 0.04 eV, respectively, suggesting the superiority of PtBV as a catalyst for low temperature CO oxidation.

  17. Ternary Pt9RhFex Nanoscale Alloys as Highly Efficient Catalysts with Enhanced Activity and Excellent CO-Poisoning Tolerance for Ethanol Oxidation.

    Science.gov (United States)

    Wang, Peng; Yin, Shibin; Wen, Ying; Tian, Zhiqun; Wang, Ningzhang; Key, Julian; Wang, Shuangbao; Shen, Pei Kang

    2017-03-22

    To address the problems of high cost and poor stability of anode catalysts in direct ethanol fuel cells (DEFCs), ternary nanoparticles Pt 9 RhFe x (x = 1, 3, 5, 7, and 9) supported on carbon powders (XC-72R) have been synthesized via a facile method involving reduction by sodium borohydride followed by thermal annealing in N 2 at ambient pressure. The catalysts are physically characterized by X-ray diffraction, scanning transmission electron microscopy, and X-ray photoelectron spectroscopy, and their catalytic performance for the ethanol oxidation reaction (EOR) is evaluated by cyclic and linear scan voltammetry, CO-stripping voltammograms, and chronopotentiometry. All the Pt 9 RhFe x /C catalysts of different atomic ratios produce high EOR catalytic activity. The catalyst of atomic ratio composition 9:1:3 (Pt/Rh/Fe) has the highest activity and excellent CO-poisoning tolerance. Moreover, the enhanced EOR catalytic activity on Pt 9 RhFe 3 /C when compared to Pt 9 Rh/C, Pt 3 Fe/C, and Pt/C clearly demonstrates the presence of Fe improves catalytic performance. Notably, the onset potential for CO oxidation on Pt 9 RhFe 3 /C (0.271 V) is ∼55, 75, and 191 mV more negative than on Pt 9 Rh/C (0.326 V), Pt 3 Fe/C (0.346 V), and Pt/C (0.462 V), respectively, which implies the presence of Fe atoms dramatically improves CO-poisoning tolerance. Meanwhile, compared to the commercial PtRu/C catalyst, the peak potential on Pt 9 RhFe 3 /C for CO oxidation was just slightly changed after several thousand cycles, which shows high stability against the potential cycling. The possible mechanism by which Fe and Rh atoms facilitate the observed enhanced performance is also considered herein, and we conclude Pt 9 RhFe 3 /C offers a promising anode catalyst for direct ethanol fuel cells.

  18. Morphology-Tuned Synthesis of Nickel Cobalt Selenides as Highly Efficient Pt-Free Counter Electrode Catalysts for Dye-Sensitized Solar Cells.

    Science.gov (United States)

    Qian, Xing; Li, Hongmei; Shao, Li; Jiang, Xiancai; Hou, Linxi

    2016-11-02

    In this work, morphology-tuned ternary nickel cobalt selenides based on different Ni/Co molar ratios have been synthesized via a simple precursor conversion method and used as counter electrode (CE) materials for dye-sensitized solar cells (DSSCs). The experimental facts and mechanism analysis clarified the possible growth process of product. It can be found that the electrochemical performance and structures of ternary nickel cobalt selenides can be optimized by tuning the Ni/Co molar ratio. Benefiting from the unique morphology and tunable composition, among the as-prepared metal selenides, the electrochemical measurements showed that the ternary nickel cobalt selenides exhibited a more superior electrocatalytic activity in comparison with binary Ni and Co selenides. In particular, the three-dimensional dandelion-like Ni 0.33 Co 0.67 Se microspheres delivered much higher power conversion efficiency (9.01%) than that of Pt catalyst (8.30%) under AM 1.5G irradiation.

  19. Pt-Ni and Pt-Co Catalyst Synthesis Route for Fuel Cell Applications

    Science.gov (United States)

    Firdosy, Samad A.; Ravi, Vilupanur A.; Valdez, Thomas I.; Kisor, Adam; Narayan, Sri R.

    2013-01-01

    Oxygen reduction reactions (ORRs) at the cathode are the rate-limiting step in fuel cell performance. The ORR is 100 times slower than the corresponding hydrogen oxidation at the anode. Speeding up the reaction at the cathode will improve fuel cell efficiency. The cathode material is generally Pt powder painted onto a substrate (e.g., graphite paper). Recent efforts in the fuel cell area have focused on replacing Pt with Pt-X alloys (where X = Co, Ni, Zr, etc.) in order to (a) reduce cost, and (b) increase ORR rates. One of these strategies is to increase ORR rates by reducing the powder size, which would result in an increase in the surface area, thereby facilitating faster reaction rates. In this work, a process has been developed that creates Pt-Ni or Pt-Co alloys that are finely divided (on the nano scale) and provide equivalent performance at lower Pt loadings. Lower Pt loadings will translate to lower cost. Precursor salts of the metals are dissolved in water and mixed. Next, the salt mixtures are dried on a hot plate. Finally, the dried salt mixture is heattreated in a furnace under flowing reducing gas. The catalyst powder is then used to fabricate a membrane electrode assembly (MEA) for electrochemical performance testing. The Pt- Co catalyst-based MEA showed comparable performance to an MEA fabri cated using a standard Pt black fuel cell catalyst. The main objective of this program has been to increase the overall efficiencies of fuel cell systems to support power for manned lunar bases. This work may also have an impact on terrestrial programs, possibly to support the effort to develop a carbon-free energy source. This catalyst can be used to fabricate high-efficiency fuel cell units that can be used in space as regenerative fuel cell systems, and terrestrially as primary fuel cells. Terrestrially, this technology will become increasingly important when transition to a hydrogen economy occurs.

  20. Pd@Pt Core–Shell Nanoparticles with Branched Dandelion-like Morphology as Highly Efficient Catalysts for Olefin Reduction

    Science.gov (United States)

    A facile synthesis based on the addition of ascorbic acid to a mixture of Na2PdCl4, K2PtCl6, and Pluronic P123 results in highly branched core–shell nanoparticles (NPs) with a micro–mesoporous dandelion-like morphology comprising Pd core and Pt shell. The slow reduction kinetics ...

  1. Enhanced activity of Pt/CNTs anode catalyst for direct methanol fuel cells using Ni2P as co-catalyst

    Science.gov (United States)

    Li, Xiang; Luo, Lanping; Peng, Feng; Wang, Hongjuan; Yu, Hao

    2018-03-01

    The direct methanol fuel cell is a promising energy conversion device because of the utilization of the state-of-the-art platinum (Pt) anode catalyst. In this work, novel Pt/Ni2P/CNTs catalysts were prepared by the H2 reduction method. It was found that the activity and stability of Pt for methanol oxidation reaction (MOR) could be significantly enhanced while using nickel phosphide (Ni2P) nanoparticles as co-catalyst. X-ray photoelectron spectroscopy revealed that the existence of Ni2P affected the particle size and electronic distribution of Pt obviously. Pt/CNTs catalyst, Pt/Ni2P/CNTs catalysts with different Ni2P amount were synthesized, among which Pt/6%Ni2P/CNTs catalyst exhibited the best MOR activity of 1400 mAmg-1Pt, which was almost 2.5 times of the commercial Pt/C-JM catalyst. Moreover, compared to other Pt-based catalysts, this novel Pt/Ni2P/CNTs catalyst also exhibited higher onset current density and better steady current density. The result of this work may provide positive guidance to the research on high efficiency and stability of Pt-based catalyst for direct methanol fuel cells.

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

    Science.gov (United States)

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

    2013-11-01

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

  3. Reclaim/recycle of Pt/C catalysts for PEMFC

    International Nuclear Information System (INIS)

    Zhao, Jishi; He, Xiangming; Tian, Jianhua; Wan, Chunrong; Jiang, Changyin

    2007-01-01

    Platinum was reclaimed from Pt/C catalysts of the PEMFC by drying the degraded Pt/C catalysts at 80 o C for 3 h, followed by sintering at 600 o C for 6 h, dissolution by aqua fortis, purification with hydrochloric acid, reduction and filtration, successively. Pt/C catalysts were prepared again from the reclaimed Pt by two proposed processes, e.g., pH value control process and mass control process. The fuel cell with recycled catalysts presented a power density of over 0.18 W cm -2 . The reclaiming of Pt/C catalysts is a potential way for recycling Pt for PEMFC, reducing the cost of PEMFC

  4. Kinetically Controlled Synthesis of Pt-Based One-Dimensional Hierarchically Porous Nanostructures with Large Mesopores as Highly Efficient ORR Catalysts.

    Science.gov (United States)

    Fu, Shaofang; Zhu, Chengzhou; Song, Junhua; Engelhard, Mark H; Xia, Haibing; Du, Dan; Lin, Yuehe

    2016-12-28

    Rational design and construction of Pt-based porous nanostructures with large mesopores have triggered significant considerations because of their high surface area and more efficient mass transport. Hydrochloric acid-induced kinetically controlled reduction of metal precursors in the presence of soft template F-127 and hard template tellurium nanowires has been successfully demonstrated to construct one-dimensional hierarchical porous PtCu alloy nanostructures with large mesopores. Moreover, the electrochemical experiments demonstrated that the PtCu hierarchically porous nanostructures synthesized under optimized conditions exhibit enhanced electrocatalytic performance for oxygen reduction reaction in acid media.

  5. Kinetically Controlled Synthesis of Pt-Based One-Dimensional Hierarchically Porous Nanostructures with Large Mesopores as Highly Efficient ORR Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Fu, Shaofang; Zhu, Chengzhou; Song, Junhua; Engelhard, Mark H.; Xia, Haibing; Du, Dan; Lin, Yuehe

    2016-12-28

    Rational design and construction of Pt-based porous nanostructures with large mesopores have triggered significant considerations because of their high surface area and more efficient mass transport. Hydrochloric acid-induced kinetic reduction of metal precursors in the presence of soft template F-127 and hard template tellurium nanowires has been successfully demonstrated to construct one-dimensional hierarchical porous PtCu alloy nanostructures with large mesopores. Moreover, the electrochemical experiments demonstrated that the resultant PtCu hierarchically porous nanostructures with optimized composition exhibit enhanced electrocatalytic performance for oxygen reduction reaction.

  6. Efficient decomposition of formaldehyde at room temperature over Pt/honeycomb ceramics with ultra-low Pt content.

    Science.gov (United States)

    Nie, Longhui; Zheng, Yingqiu; Yu, Jiaguo

    2014-09-14

    Pt/honeycomb ceramic (Pt/HC) catalysts with ultra-low Pt content (0.005-0.055 wt%) were for the first time prepared by an impregnation of honeycomb ceramics with Pt precursor and NaBH4-reduction combined method. The microstructures, morphologies and textural properties of the resulting samples were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), and transmission electron microscopy (TEM). The obtained Pt/HC catalysts were used for catalytic oxidative decomposition of formaldehyde (HCHO) at room temperature. It was found that the as-prepared Pt/HC catalysts can efficiently decompose HCHO in air into CO2 and H2O at room temperature. The catalytic activity of the Pt/HC catalysts increases with increasing the Pt loading in the range of 0.005-0.013 wt%, and the further increase of the Pt loading does not obviously improve catalytic activity. From the viewpoint of cost and catalytic performance, 0.013 wt% Pt loading is the optimal Pt loading amount, and the Pt/HC catalyst with 0.013 wt% Pt loading also exhibited good catalytic stability. Considering practical applications, this work will provide new insights into the low-cost and large-scale fabrication of advanced catalytic materials for indoor air purification.

  7. Design criteria for stable Pt/C fuel cell catalysts

    Directory of Open Access Journals (Sweden)

    Josef C. Meier

    2014-01-01

    Full Text Available Platinum and Pt alloy nanoparticles supported on carbon are the state of the art electrocatalysts in proton exchange membrane fuel cells. To develop a better understanding on how material design can influence the degradation processes on the nanoscale, three specific Pt/C catalysts with different structural characteristics were investigated in depth: a conventional Pt/Vulcan catalyst with a particle size of 3–4 nm and two Pt@HGS catalysts with different particle size, 1–2 nm and 3–4 nm. Specifically, Pt@HGS corresponds to platinum nanoparticles incorporated and confined within the pore structure of the nanostructured carbon support, i.e., hollow graphitic spheres (HGS. All three materials are characterized by the same platinum loading, so that the differences in their performance can be correlated to the structural characteristics of each material. The comparison of the activity and stability behavior of the three catalysts, as obtained from thin film rotating disk electrode measurements and identical location electron microscopy, is also extended to commercial materials and used as a basis for a discussion of general fuel cell catalyst design principles. Namely, the effects of particle size, inter-particle distance, certain support characteristics and thermal treatment on the catalyst performance and in particular the catalyst stability are evaluated. Based on our results, a set of design criteria for more stable and active Pt/C and Pt-alloy/C materials is suggested.

  8. Pt based anode catalysts for direct ethanol fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Weijiang; Zhou, Zhenhua; Song, Shuqin; Li, Wenzhen; Sun, Gongquan; Xin, Qin [Direct Alcohol Fuel Cell Laboratory, Dalian Institute of Chemical Physics, CAS, P.O. Box 110, Dalian 116023 (China); Tsiakaras, Panagiotis [Department of Mechanical and Industrial Engineering, University of Thessalia, Pedion Areos, GR 38334 Volos (Greece) 7

    2003-11-10

    In the present work several Pt-based anode catalysts supported on carbon XC-72R were prepared with a novel method and characterized by means of XRD, TEM and XPS analysis. It was found that all these catalysts are consisted of uniform nanosized particles with sharp distribution and Pt lattice parameter decreases with the addition of Ru or Pd and increases with the addition of Sn or W. Cyclic voltammetry (CV) measurements and single direct ethanol fuel cell (DEFC) tests jointly showed that the presence of Sn, Ru and W enhances the activity of Pt towards ethanol electro-oxidation in the following order: Pt{sub 1}Sn{sub 1}/C>Pt{sub 1}Ru{sub 1}/C>Pt{sub 1}W{sub 1}/C>Pt{sub 1}Pd{sub 1}/C>Pt/C. Moreover, Pt{sub 1}Ru{sub 1}/C further modified by W and Mo showed improved ethanol electro-oxidation activity, but its DEFC performance was found to be inferior to that measured for Pt{sub 1}Sn{sub 1}/C. Under this respect, several PtSn/C catalysts with different Pt/Sn atomic ratio were also identically prepared and characterized and their direct ethanol fuel cell performances were evaluated. It was found that the single direct ethanol fuel cell having Pt{sub 1}Sn{sub 1}/C or Pt{sub 3}Sn{sub 2}/C or Pt{sub 2}Sn{sub 1}/C as anode catalyst showed better performances than those with Pt{sub 3}Sn{sub 1}/C or Pt{sub 4}Sn{sub 1}/C. It was also found that the latter two cells exhibited higher performances than the single cell using Pt{sub 1}Ru{sub 1}/C, which is exclusively used in PEMFC as anode catalyst for both methanol electro-oxidation and CO-tolerance. This distinct difference in DEFC performance between the catalysts examined here would be attributed to the so-called bifunctional mechanism and to the electronic interaction between Pt and additives. It is thought that an amount of -OH{sub ads}, an amount of surface Pt active sites and the conductivity effect of PtSn/C catalysts would determine the activity of PtSn/C with different Pt/Sn ratios. At lower temperature values or at low

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

    Directory of Open Access Journals (Sweden)

    A.B. da Silva

    1998-06-01

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

  10. Pt/Ceria-based Catalysts for Small Alcohol Electrooxidation

    Science.gov (United States)

    Menendez-Mora, Christian L.

    High emissions of fossil-based energy sources have led to scientists around the world to develop new alternatives for the future. In this sense, fuel cells are a remarkable and promising energy option with less environmental impact. The most used fuels for this technology are hydrogen and small chain alcohols, which can be oxidized to transform their chemical energy into electrical power. To do this, fuel cells need catalysts that will act as an active surface where the oxidation can take place. The problem with platinum catalysts is its possible CO poisoning with intermediates that are produced before the complete oxidation of alcohol to CO2. Different approaches have been taken to try to resolve this issue. In this case, cerium oxide (ceria) was selected as a co-catalyst to mitigate the effect of CO poisoning of platinum. Ceria is a compound that has the ability to work as an "oxygen tank" and can donate oxygen to carbon monoxide that is strongly adsorbed at platinum surface to produce CO2 (carbon dioxide), regenerating the Pt surface for further alcohol oxidation. Therefore, enhancing the current density as well as the power output of a fuel cell. First, an occlusion deposition technique was used to prepare platinum/ceria composite electrodes and tested them towards small chain alcohol oxidation such as methanol oxidation reaction in acidic and alkaline media. The preliminary results demonstrated that the Pt/ceria electrodes were more efficient towards methanol electrooxidation when compared to Pt electrodes. This enhancement was attributed to the presence of ceria. A second preparation method was selected for the synthesis of ceria/Pt catalysts. In this case, a hydrothermal method was used and the catalysis were studied for the effect of MeOH, EtOH and n-BuOH oxidation. The observed effect was that electrodes made of Pt/Pt:CeO2-x showed better catalytic effect than Pt/ceria and platinum electrodes. Moreover, a comparison between ceria nanorods versus

  11. Hydrodeoxygenation of Guaiacol Over Pt/Al-SBA-15 Catalysts.

    Science.gov (United States)

    Yu, Mi Jin; Park, Sung Hoon; Jeon, Jong-Ki; Ryu, Changkook; Sohn, Jung Min; Kim, Sang Chai; Park, Young-Kwon

    2015-01-01

    Upgrading of bio-oil through catalytic hydrodeoxygenation (HDO) reaction was investigated for guaiacol as a model compound. A batch reactor was used for the reaction condition of 40 bar and 250 degrees C. The target product was cyclohexane. Pt/Al-SBA-15 with the Si/Al ratios of 20, 40, and 80 and Pt/HZSM-5 were used as the catalyst. The SBA-15 catalysts were characterized by N2 adsorption-desorption, X-ray diffraction analysis, and temperature programmed desorption of ammonia. The order of cyclohexane yield was Pt/Al-SBA-15 (Si/Al = 20) > Pt/Al-SBA-15(40) > Pt/Al-SBA-15 (80), indicating that the quantity of acid sites plays an important role in the HDO reaction. On the other hand, Pt/HZSM-5 led to a very low cyclohexane yield, in spite of its abundant strong acid sites, due to its small pore size.

  12. Catalysts synthesized by selective deposition of Fe onto Pt for the water-gas shift reaction

    Energy Technology Data Exchange (ETDEWEB)

    Aragao, Isaias Barbosa; Ro, Insoo; Liu, Yifei; Ball, Madelyn; Huber, George W.; Zanchet, Daniela; Dumesic, James A.

    2018-03-01

    FePt bimetallic catalysts with intimate contact between the two metals were synthesized by controlled surface reactions (CSR) of (cyclohexadiene)iron tricarbonyl with hydrogen-treated supported Pt nanoparticles. Adsorption of the iron precursor on a Pt/SiO2 catalyst was studied, showing that the Fe loading could be increased by performing multiple CSR cycles, and the efficiency of this process was linked to the renewal of adsorption sites by a reducing pretreatment. The catalytic activity of these bimetallic catalysts for the water gas shift reaction was improved due to promotion by iron, likely linked to H2O activation on FeOx species at or near the Pt surface, mostly in the (II) oxidation state.

  13. Chemisorption studies of Pt/SnO2 catalysts

    Science.gov (United States)

    Brown, Kenneth G.; Ohorodnik, Susan K.; Vannorman, John D.; Schryer, Jacqueline; Upchurch, Billy T.; Schryer, David R.

    1990-01-01

    The low temperature CO oxidation catalysts that are being developed and tested at NASA-Langley are fairly unique in their ability to efficiently oxidize CO at low temperatures (approx. 303 K). The bulk of the reaction data that has been collected in the laboratory has been determined using plug flow reactors with a low mass of Pt/SnO2/SiO2 catalyst (approx. 0.1 g) and a modest flow rate (5 to 10 sc sm). The researchers have previously characterized the surface solely in terms of N2 BET surface areas. These surface areas have not been that indicative of reaction rate. Indeed, some of the formulations with high BET surface area have yielded lower reaction rates than those with lower BET surface areas. As a result researchers began a program of determining the chemisorption of the various species involved in the reaction; CO, O2 and CO2. Such a determination of will lead to a better understanding of the mechanism and overall kinetics of the reaction. The pulsed-reactor technique, initially described by Freel, is used to determine the amount of a particular molecule that is adsorbed on the catalyst. Since there is some reaction of CO with the surface to produce CO2, the pulsed reactor had to be coupled with a gas chromatograph in order to distinguish between the loss of CO that is due to adsorption by the surface and the loss that is due to reaction with the surface.

  14. Particle size dependence of CO tolerance of anode PtRu catalysts for polymer electrolyte fuel cells

    Science.gov (United States)

    Yamanaka, Toshiro; Takeguchi, Tatsuya; Wang, Guoxiong; Muhamad, Ernee Noryana; Ueda, Wataru

    An anode catalyst for a polymer electrolyte fuel cell must be CO-tolerant, that is, it must have the function of hydrogen oxidation in the presence of CO, because hydrogen fuel gas generated by the steam reforming process of natural gas contains a small amount of CO. In the present study, PtRu/C catalysts were prepared with control of the degree of Pt-Ru alloying and the size of PtRu particles. This control has become possible by a new method of heat treatment at the final step in the preparation of catalysts. The CO tolerances of PtRu/C catalysts with the same degree of Pt-Ru alloying and with different average sizes of PtRu particles were thus compared. Polarization curves were obtained with pure H 2 and CO/H 2 (CO concentrations of 500-2040 ppm). It was found that the CO tolerance of highly dispersed PtRu/C (high dispersion (HD)) with small PtRu particles was much higher than that of poorly dispersed PtRu/C (low dispersion (LD)) with large metal particles. The CO tolerance of PtRu/C (HD) was higher than that of any commercial PtRu/C. The high CO tolerance of PtRu/C (HD) is thought to be due to efficient concerted functions of Pt, Ru, and their alloy.

  15. 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

  16. Pt/SnO2-based CO-oxidation catalysts for long-life closed-cycle CO2 lasers

    Science.gov (United States)

    Schryer, David R.; Upchurch, Billy T.; Hess, Robert V.; Wood, George M.; Sidney, Barry D.; Miller, Irvin M.; Brown, Kenneth G.; Vannorman, John D.; Schryer, Jacqueline; Brown, David R.

    1990-01-01

    Noble-metal/tin-oxide based catalysts such as Pt/SnO2 have been shown to be good catalysts for the efficient oxidation of CO at or near room temperature. These catalysts require a reductive pretreatment and traces of hydrogen or water to exhibit their full activity. Addition of Palladium enhances the activity of these catalysts with about 15 to 20 percent Pt, 4 percent Pd, and the balance SnO2 being an optimum composition. Unfortunately, these catalysts presently exhibit significant decay due in part to CO2 retention, probably as a bicarbonate. Research on minimizing the decay in activity of these catalysts is currently in progress. A proposed mechanism of CO oxidation on Pt/SnO2-based catalysts has been developed and is discussed.

  17. Single-Atom Pt as Co-Catalyst for Enhanced Photocatalytic H2 Evolution.

    Science.gov (United States)

    Li, Xiaogang; Bi, Wentuan; Zhang, Lei; Tao, Shi; Chu, Wangsheng; Zhang, Qun; Luo, Yi; Wu, Changzheng; Xie, Yi

    2016-03-23

    Isolated single-atom platinum (Pt) embedded in the sub-nanoporosity of 2D g-C3 N4 as a new form of co-catalyst is reported. The highly stable single-atom co-catalyst maximizes the atom efficiency and alters the surface trap states of g-C3 N4 , leading to significantly enhanced photocatalytic H2 evolution activity, 8.6 times higher than that of Pt nanoparticles and up to 50 times that for bare g-C3 N4 . © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Metal Phosphate-Supported Pt Catalysts for CO Oxidation

    Directory of Open Access Journals (Sweden)

    Xiaoshuang Qian

    2014-12-01

    Full Text Available Oxides (such as SiO2, TiO2, ZrO2, Al2O3, Fe2O3, CeO2 have often been used to prepare supported Pt catalysts for CO oxidation and other reactions, whereas metal phosphate-supported Pt catalysts for CO oxidation were rarely reported. Metal phosphates are a family of metal salts with high thermal stability and acid-base properties. Hydroxyapatite (Ca10(PO46(OH2, denoted as Ca-P-O here also has rich hydroxyls. Here we report a series of metal phosphate-supported Pt (Pt/M-P-O, M = Mg, Al, Ca, Fe, Co, Zn, La catalysts for CO oxidation. Pt/Ca-P-O shows the highest activity. Relevant characterization was conducted using N2 adsorption-desorption, inductively coupled plasma (ICP atomic emission spectroscopy, X-ray diffraction (XRD, transmission electron microscopy (TEM, CO2 temperature-programmed desorption (CO2-TPD, X-ray photoelectron spectroscopy (XPS, and H2 temperature-programmed reduction (H2-TPR. This work furnishes a new catalyst system for CO oxidation and other possible reactions.

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

    International Nuclear Information System (INIS)

    Naeem, R.; Ahmed, R.; Ansari, M.S.

    2013-01-01

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

  20. Rapid and facile CuCl assistant synthesis of PtCu3 nanoframes as efficient catalysts for electroxidation of methanol

    Science.gov (United States)

    Bai, Lei; Bai, Yuwei

    2018-02-01

    Hollow-structured nanomaterials generally showed enhanced catalytic abilities due to their high utilization. In this work, a general method for the synthesis of PtCu3 nanoframes was reported with the employment of hexadecyltrimethylammonium chloride (CTAC), copper(I) chloride, and various kinds of platinum precursors such as K2PtCl6, H2PtCl6, and Pt(acac)2. It was revealed that the presence of CTAC was crucial for the formation of frame structures. On the one hand, CTAC could act as a structure director, and on the other hand, the galvanic replacement and etching effect of the chloride ions together with oxygen was also responsible for the formation of the frame structure. A similar effect was also evidenced in the case of hexadecyltrimethylammonium bromide. Finally, the as-obtained PtCu3 nanoframes demonstrated high catalytic abilities in the oxidation of methanol as a model reaction. [Figure not available: see fulltext.

  1. 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.

  2. CO oxidation on PtSn nanoparticle catalysts occurs at the interface of Pt and Sn oxide domains formed under reaction conditions

    KAUST Repository

    Michalak, William D.

    2014-04-01

    The barrier to CO oxidation on Pt catalysts is the strongly bound adsorbed CO, which inhibits O2 adsorption and hinders CO2 formation. Using reaction studies and in situ X-ray spectroscopy with colloidally prepared, monodisperse ∼2 nm Pt and PtSn nanoparticle catalysts, we show that the addition of Sn to Pt provides distinctly different reaction sites and a more efficient reaction mechanism for CO oxidation compared to pure Pt catalysts. To probe the influence of Sn, we intentionally poisoned the Pt component of the nanoparticle catalysts using a CO-rich atmosphere. With a reaction environment comprised of 100 Torr CO and 40 Torr O2 and a temperature range between 200 and 300 C, Pt and PtSn catalysts exhibited activation barriers for CO2 formation of 133 kJ/mol and 35 kJ/mol, respectively. While pure Sn is readily oxidized and is not active for CO oxidation, the addition of Sn to Pt provides an active site for O2 adsorption that is important when Pt is covered with CO. Sn oxide was identified as the active Sn species under reaction conditions by in situ ambient pressure X-ray photoelectron spectroscopy measurements. While chemical signatures of Pt and Sn indicated intermixed metallic components under reducing conditions, Pt and Sn were found to reversibly separate into isolated domains of Pt and oxidic Sn on the nanoparticle surface under reaction conditions of 100 mTorr CO and 40 mTorr O2 between temperatures of 200-275 C. Under these conditions, PtSn catalysts exhibited apparent reaction orders in O2 for CO 2 production that were 0.5 and lower with increasing partial pressures. These reaction orders contrast the first-order dependence in O 2 known for pure Pt. The differences in activation barriers, non-first-order dependence in O2, and the presence of a partially oxidized Sn indicate that the enhanced activity is due to a reaction mechanism that occurs at a Pt/Sn oxide interface present at the nanoparticle surface. © 2014 Published by Elsevier Inc.

  3. Pt, Re and Pt-Re incorporation in sulfated zirconia as catalysts for n-pentane isomerization

    International Nuclear Information System (INIS)

    Aboul-Gheit, A.K.; El-Desouki, D.S.; Abdel-Hamid, S.M.; Ghoneim, S.A.; Ibrahim, A.H.; Gad, F.K.; Abdel-Aleem, G.M.

    2010-01-01

    Two groups of modified Sulfated Zirconia (S Z) catalysts were prepared by the sol-gel method. The first group was modified by four different concentrations of Pt metal (0.15, 0.30, 0.45 and 0.60 wt %), whereas the second group contained Pt-Re combinations on SZ. All the prepared catalysts were characterized by XRD, TPR, TEM, TGA, IR spectroscopy as well as surface properties using the BET method. The catalytic activity of the catalysts was examined for the hydro isomerization of n-pentane to iso-pentane. The catalytic activity was found to increase with increasing Pt concentration in the mono metallic catalysts. The combination of Re ion with Pt on SZ results in significant changes in the characters and activities of the catalysts. The 0.45 wt % Pt + 0.15 wt % Re/SZ catalyst exhibited the highest selective compared to other metal ratios investigated

  4. Pt atoms stabilized on hexagonal boron nitride as efficient single-atom catalysts for CO oxidation: A first-principles investigation

    KAUST Repository

    Liu, Xin; Duan, Ting; Meng, Changgong; Han, Yu

    2015-01-01

    Taking CO oxidation as a probe, we investigated the electronic structure and reactivity of Pt atoms stabilized by vacancy defects on hexagonal boron nitride (h-BN) by first-principles-based calculations. As a joint effect of the high reactivity

  5. Reverse microemulsion prepared Ni–Pt catalysts for methane cracking to produce COx-free hydrogen

    KAUST Repository

    Zhou, Lu

    2017-09-08

    A monodispersed 15 nm Ni9Pt1 catalyst synthesized via a reverse microemulsion method, shows a lower activation energy than both Ni and Pt catalysts during the methane cracking reaction. Thanks to the synergic effect of Ni–Pt alloy, this catalyst presents a stable H2 formation rate at 700 °C, and forms carbon nanotubes, anchoring the catalyst particles on top.

  6. Reverse microemulsion prepared Ni–Pt catalysts for methane cracking to produce COx-free hydrogen

    KAUST Repository

    Zhou, Lu; Harb, Moussab; Enakonda, Linga Reddy; Al Mana, Noor; Hedhili, Mohamed N.; Basset, Jean-Marie

    2017-01-01

    A monodispersed 15 nm Ni9Pt1 catalyst synthesized via a reverse microemulsion method, shows a lower activation energy than both Ni and Pt catalysts during the methane cracking reaction. Thanks to the synergic effect of Ni–Pt alloy, this catalyst presents a stable H2 formation rate at 700 °C, and forms carbon nanotubes, anchoring the catalyst particles on top.

  7. Effect of hydrogen and propylene on the hydrogen peroxide decomposition over Pt, PtO and Au catalysts

    NARCIS (Netherlands)

    Kertalli, E.; Schouten, J.C.; Nijhuis, T.A.

    2017-01-01

    The decomposition of hydrogen peroxide (H2O2) on Pt, PtO and Au catalysts has been investigated in the presence of nitrogen, propylene and hydrogen. H2O2 formation on the catalyst is known to be a key intermediate step for the direct synthesis of propylene oxide (PO) from hydrogen, propylene and

  8. Efficient Aerobic Oxidation of Cyclohexane to KA Oil Catalyzed by Pt ...

    Indian Academy of Sciences (India)

    127, No. 7, July 2015, pp. 1167–1172. c Indian Academy of Sciences. ... The catalyst was used for the partial oxidation of cyclohexane in a Parr type reactor. It was found that Pt-Sn supported on MWCNTs can act as an efficient catalyst for the partial ... version ratio with high selectivity for KA oil in a liquid ... These gases.

  9. 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)

  10. Pt/Cr and Pt/Ni catalysts for oxygen reduction reaction: to alloy or not to alloy?

    Science.gov (United States)

    Escaño, Mary Clare; Gyenge, Elod; Nakanishi, Hiroshi; Kasai, Hideaki

    2011-04-01

    Bimetallic systems such as Pt-based alloys or non-alloys have exhibited interesting catalytic properties but pose a major challenge of not knowing a priori how the electronic and chemical properties will be modified relative to the parent metals. In this work, we present the origin of the changes in the reactivity of Pt/Cr and Pt/Ni catalysts, which have been of wide interest in fuel cell research. Using spin-polarized density functional theory calculations, we have shown that the modification of Pt surface reactivity in Pt/Ni is purely of geometric origin (strain). We have also found that the Pt-Ni bonding is very weak, which explains the observed instability of Pt-Ni catalysts under electrochemical measurements. On the other hand, Pt/Cr systems are governed by strong ligand effect (metal-metal interaction), which explains the experimentally observed reactivity dependence on the relative composition of the alloying components. The general characteristics of the potential energy curves for O2 dissociative adsorption on the bimetallic systems and the pure Pt clarify why the d-band center still works for Pt/Cr despite the strong Pt-Cr bonding and high spin polarization of Pt d-states. On the basis of the above clarifications, viable Pt-Cr and Pt-Ni structures, which involve nano-sized alloys and non-alloy bulk catalyst, which may strike higher than the currently observed oxidation reduction reaction activity are proposed.

  11. Electro-oxidation of ethanol and ethylene glycol on carbon-supported nano-Pt and -PtRu catalyst in acid solution

    International Nuclear Information System (INIS)

    Chatterjee, Moitrayee; Chatterjee, Abhik; Ghosh, Susanta; Basumallick, I.

    2009-01-01

    Present paper reports kinetics of electro-oxidation of ethanol (EtOH) and ethylene glycol (EG) onto Pt and PtRu nanocatalysts of different compositions in the temperature range of 298-318 K. These catalysts have been characterized by SEM, EDX, XRD, CV and amperometry. It has been observed that apparent activation energies for oxidation of EtOH and EG pass through a minimum at about 15-20 at.% of Ru in the PtRu alloy catalysts. Anodic peak current vs. composition curve also shows a maximum around this composition. The results have been explained by a geometric model, which proposes requirement of an ensemble of three Pt atoms with an adjacent Ru atom onto PtRu surface for an efficient electro-oxidation of EtOH or EG. This is further supported from statistical data analysis of probability of occurrence of such ensembles onto PtRu alloy surface. Present results also suggest that electro-oxidation of EG onto nano-PtRu catalyst surfaces follows a different path from that of EtOH at alloy composition less than 15 at.% of Ru.

  12. Electro-oxidation of ethanol and ethylene glycol on carbon-supported nano-Pt and -PtRu catalyst in acid solution

    Energy Technology Data Exchange (ETDEWEB)

    Chatterjee, Moitrayee; Chatterjee, Abhik; Ghosh, Susanta [Electrochemical Laboratory, Department of Chemistry, Visva-Bharati University, Santiniketan 731235 (India); Basumallick, I., E-mail: ibasumallick@yahoo.co.u [Electrochemical Laboratory, Department of Chemistry, Visva-Bharati University, Santiniketan 731235 (India)

    2009-12-01

    Present paper reports kinetics of electro-oxidation of ethanol (EtOH) and ethylene glycol (EG) onto Pt and PtRu nanocatalysts of different compositions in the temperature range of 298-318 K. These catalysts have been characterized by SEM, EDX, XRD, CV and amperometry. It has been observed that apparent activation energies for oxidation of EtOH and EG pass through a minimum at about 15-20 at.% of Ru in the PtRu alloy catalysts. Anodic peak current vs. composition curve also shows a maximum around this composition. The results have been explained by a geometric model, which proposes requirement of an ensemble of three Pt atoms with an adjacent Ru atom onto PtRu surface for an efficient electro-oxidation of EtOH or EG. This is further supported from statistical data analysis of probability of occurrence of such ensembles onto PtRu alloy surface. Present results also suggest that electro-oxidation of EG onto nano-PtRu catalyst surfaces follows a different path from that of EtOH at alloy composition less than 15 at.% of Ru.

  13. The kinetics and mechanism of methanol oxidation on Pt and PtRu catalysts in alkaline and acid media

    Directory of Open Access Journals (Sweden)

    JELENA LOVIC

    2007-07-01

    Full Text Available The kinetic of methanol electrochemical oxidation for a series of platinum and platinum–ruthenium catalysts was investigated. A correlation between the beginning of OHad adsorption and methanol oxidation was demonstarated on Pt single crystals and Pt nanocatalyst. The activity of the nano-structured Pt catalyst was compared with single crystal platinum electrodes assuming the Kinoshita model of nanoparticles. The ruthenium-containing catalysts shifted the onset of methanol oxidation to more negative potentials. The effect was more pronounced in acid than in alkaline media. Based on the established diagnostic criteria, the reaction between COad and OHad species according to the Langmuir–Hinshelwood mechanism was proposed as the rate determining step in alkaline and acid media on Pt and PtRu catalysts.

  14. Catalyst Architecture for Stable Single Atom Dispersion Enables Site-Specific Spectroscopic and Reactivity Measurements of CO Adsorbed to Pt Atoms, Oxidized Pt Clusters, and Metallic Pt Clusters on TiO2.

    Science.gov (United States)

    DeRita, Leo; Dai, Sheng; Lopez-Zepeda, Kimberly; Pham, Nicholas; Graham, George W; Pan, Xiaoqing; Christopher, Phillip

    2017-10-11

    Oxide-supported precious metal nanoparticles are widely used industrial catalysts. Due to expense and rarity, developing synthetic protocols that reduce precious metal nanoparticle size and stabilize dispersed species is essential. Supported atomically dispersed, single precious metal atoms represent the most efficient metal utilization geometry, although debate regarding the catalytic activity of supported single precious atom species has arisen from difficulty in synthesizing homogeneous and stable single atom dispersions, and a lack of site-specific characterization approaches. We propose a catalyst architecture and characterization approach to overcome these limitations, by depositing ∼1 precious metal atom per support particle and characterizing structures by correlating scanning transmission electron microscopy imaging and CO probe molecule infrared spectroscopy. This is demonstrated for Pt supported on anatase TiO 2 . In these structures, isolated Pt atoms, Pt iso , remain stable through various conditions, and spectroscopic evidence suggests Pt iso species exist in homogeneous local environments. Comparing Pt iso to ∼1 nm preoxidized (Pt ox ) and prereduced (Pt metal ) Pt clusters on TiO 2 , we identify unique spectroscopic signatures of CO bound to each site and find CO adsorption energy is ordered: Pt iso ≪ Pt metal atoms bonded to TiO 2 and that Pt iso exhibits optimal reactivity because every atom is exposed for catalysis and forms an interfacial site with TiO 2 . This approach should be generally useful for studying the behavior of supported precious metal atoms.

  15. Design of ultrathin Pt-Mo-Ni nanowire catalysts for ethanol electrooxidation.

    Science.gov (United States)

    Mao, Junjie; Chen, Wenxing; He, Dongsheng; Wan, Jiawei; Pei, Jiajing; Dong, Juncai; Wang, Yu; An, Pengfei; Jin, Zhao; Xing, Wei; Tang, Haolin; Zhuang, Zhongbin; Liang, Xin; Huang, Yu; Zhou, Gang; Wang, Leyu; Wang, Dingsheng; Li, Yadong

    2017-08-01

    Developing cost-effective, active, and durable electrocatalysts is one of the most important issues for the commercialization of fuel cells. Ultrathin Pt-Mo-Ni nanowires (NWs) with a diameter of ~2.5 nm and lengths of up to several micrometers were synthesized via a H 2 -assisted solution route (HASR). This catalyst was designed on the basis of the following three points: (i) ultrathin NWs with high numbers of surface atoms can increase the atomic efficiency of Pt and thus decrease the catalyst cost; (ii) the incorporation of Ni can isolate Pt atoms on the surface and produce surface defects, leading to high catalytic activity (the unique structure and superior activity were confirmed by spherical aberration-corrected electron microscopy measurements and ethanol oxidation tests, respectively); and (iii) the incorporation of Mo can stabilize both Ni and Pt atoms, leading to high catalytic stability, which was confirmed by experiments and density functional theory calculations. Furthermore, the developed HASR strategy can be extended to synthesize a series of Pt-Mo-M (M = Fe, Co, Mn, Ru, etc.) NWs. These multimetallic NWs would open up new opportunities for practical fuel cell applications.

  16. Design of Pt/Carbon Xerogel Catalysts for PEM Fuel Cells

    Directory of Open Access Journals (Sweden)

    Nathalie Job

    2015-01-01

    Full Text Available The design of efficient catalytic layers of proton exchange membrane fuel cells (PEMFCs requires the preparation of highly-loaded and highly-dispersed Pt/C catalysts. During the last few years, our work focused on the preparation of Pt/carbon xerogel electrocatalysts, starting from simple impregnation techniques that were further optimized via the strong electrostatic adsorption (SEA method to reach high dispersion and a high metal weight fraction. The SEA method, which consists of the optimization of the precursor/support electrostatic impregnation through an adequate choice of the impregnation pH with regard to the support surface chemistry, leads to very well-dispersed Pt/C samples with a maximum 8 wt.% Pt after drying and reduction under H2. To increase the metal loading, the impregnation-drying-reduction cycle of the SEA method can be repeated several times, either with fresh Pt precursor solution or with the solution recycled from the previous cycle. In each case, a high dispersion (Pt particle size ~3 nm is obtained. Finally, the procedure can be simplified by combination of the SEA technique with dry impregnation, leading to no Pt loss during the procedure.

  17. Aerobic Oxidation of Xylose to Xylaric acid in Water over Pt Catalysts.

    Science.gov (United States)

    Saha, Basudeb; Sadula, Sunitha

    2018-05-02

    Energy-efficient catalytic conversion of biomass intermediates to functional chemicals can enable bio-products viable. Herein, we report an efficient and low temperature aerobic oxidation of xylose to xylaric acid, a promising bio-based chemical for the production of glutaric acid, over commercial catalysts in water. Among several heterogeneous catalysts investigated, Pt/C exhibits the best activity. Systematic variation of reaction parameters in the pH range of 2.5 to 10 suggests that the reaction is fast at higher temperatures but high C-C scission of intermediate C5-oxidized products to low carbon carboxylic acids undermines xylaric acid selectivity. The C-C cleavage is also high in basic solution. The oxidation at neutral pH and 60 C achieves the highest xylaric acid yield (64%). O2 pressure and Pt-amount have significant influence on the reactivity. Decarboxylation of short chain carboxylic acids results in formation of CO2, causing some carbon loss; however such decarboxylation is slow in the presence of xylose. The catalyst retained comparable activity, in terms of product selectivity, after five cycles with no sign of Pt leaching. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Pt/MOx/SiO2, Pt/MOx/TiO2, and Pt/MOx/Al2O3 Catalysts for CO Oxidation

    Directory of Open Access Journals (Sweden)

    Hongmei Qin

    2015-04-01

    Full Text Available Conventional supported Pt catalysts have often been prepared by loading Pt onto commercial supports, such as SiO2, TiO2, Al2O3, and carbon. These catalysts usually have simple metal-support (i.e., Pt-SiO2 interfaces. To tune the catalytic performance of supported Pt catalysts, it is desirable to modify the metal-support interfaces by incorporating an oxide additive into the catalyst formula. Here we prepared three series of metal oxide-modified Pt catalysts (i.e., Pt/MOx/SiO2, Pt/MOx/TiO2, and Pt/MOx/Al2O3, where M = Al, Fe, Co, Cu, Zn, Ba, La for CO oxidation. Among them, Pt/CoOx/SiO2, Pt/CoOx/TiO2, and Pt/CoOx/Al2O3 showed the highest catalytic activities. Relevant samples were characterized by N2 adsorption-desorption, X-ray diffraction (XRD, transmission electron microscopy (TEM, H2 temperature-programmed reduction (H2-TPR, X-ray photoelectron spectroscopy (XPS, CO temperature-programmed desorption (CO-TPD, O2 temperature-programmed desorption (O2-TPD, and CO2 temperature-programmed desorption (CO2-TPD.

  19. Porous graphene supported Pt catalysts for proton exchange membrane fuel cells

    International Nuclear Information System (INIS)

    Cheng, Kun; He, Daping; Peng, Tao; Lv, Haifeng; Pan, Mu; Mu, Shichun

    2014-01-01

    Graphene nanosheet (GNS) has a remarkably high ratio of surface area to thickness and intense inter-sheet aggregation, which heavily resist mass diffusion in vertical orientation. Here, we establish a fast-speed mass diffusion passage by creating pores in GNS, and the corresponding Pt catalyst (Pt/rPGO) displays 15.5 times mass diffusion rate than that of the pristine GNS supported Pt catalyst (Pt/rGO). Thus, the Pt/rPGO catalyst exhibits 1.5 times increase in Pt mass activity toward oxygen reduction reaction compared with the Pt/rGO. Significantly, after H 2 thermal treatment, the mass activity of the Pt/rPGO further increases to 1.9 times that of the Pt/rGO, and its electrochemical stability is also greatly improved

  20. Remarkable support effect on the reactivity of Pt/In2O3/MOx catalysts for methanol steam reforming

    Science.gov (United States)

    Liu, Xin; Men, Yong; Wang, Jinguo; He, Rong; Wang, Yuanqiang

    2017-10-01

    Effects of supports over Pt/In2O3/MOx catalysts with extremely low loading of Pt (1 wt%) and In2O3 loadings (3 wt%) are investigated for the hydrogen production of methanol steam reforming (MSR) in the temperature range of 250-400 °C. Under practical conditions without the pre-reduction, the 1Pt/3In2O3/CeO2 catalyst shows the highly efficient catalytic performance, achieving almost complete methanol conversion (98.7%) and very low CO selectivity of 2.6% at 325 °C. The supported Pt/In2O3 catalysts are characterized by means of Brunauer-Emmett-Teller (BET) surface area, X-ray diffraction (XRD), high-resolution transmission microscopy (HRTEM), temperature programmed reduction with hydrogen (H2-TPR), CO pulse chemisorption, temperature programmed desorption of methanol and water (CH3OH-TPD and H2O-TPD). These demonstrate that the nature of catalyst support of Pt/In2O3/MOx plays crucial roles in the Pt dispersion associated by the strong interaction among Pt, In2O3 and supporting materials and the surface redox properties at low temperature, and thus affects their capability to activate the reactants and determines the catalytic activity of methanol steam reforming. The superior 1Pt/3In2O3/CeO2 catalyst, exhibiting a remarkable reactivity and stability for 32 h on stream, demonstrates its potential for efficient hydrogen production of methanol steam reforming in mobile and de-centralized H2-fueled PEMFC systems.

  1. Ethanol electrooxidation on novel carbon supported Pt/SnOx/C catalysts with varied Pt:Sn ratio

    International Nuclear Information System (INIS)

    Jiang, L.; Colmenares, L.; Jusys, Z.; Sun, G.Q.; Behm, R.J.

    2007-01-01

    Novel carbon supported Pt/SnO x /C catalysts with Pt:Sn atomic ratios of 5:5, 6:4, 7:3 and 8:2 were prepared by a modified polyol method and characterized with respect to their structural properties (X-ray diffraction (XRD) and transmission electron microscopy (TEM)), chemical composition (XPS), their electrochemical properties (base voltammetry, CO ad stripping) and their electrocatalytic activity and selectivity for ethanol oxidation (ethanol oxidation reaction (EOR)). The data show that the Pt/SnO x /C catalysts are composed of Pt and tin oxide nanoparticles with an average Pt particle diameter of about 2 nm. The steady-state activity of the Pt/SnO x /C catalysts towards the EOR decreases with tin content at room temperature, but increases at 80 deg. C. On all Pt/SnO x /C catalysts, acetic acid and acetaldehyde represent dominant products, CO 2 formation contributes 1-3% for both potentiostatic and potentiodynamic reaction conditions. With increasing potential, the acetaldehyde yield decreases and the acetic acid yield increases. The apparent activation energies of the EOR increase with tin content (19-29 kJ mol -1 ), but are lower than on Pt/C (32 kJ mol -1 ). The somewhat better performance of the Pt/SnO x /C catalysts compared to alloyed PtSn x /C catalysts is attributed to the presence of both sufficiently large Pt ensembles for ethanol dehydrogenation and C-C bond splitting and of tin oxide for OH generation. Fuel cell measurements performed for comparison largely confirm the results obtained in model studies

  2. 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)

  3. SiO2 stabilized Pt/C cathode catalyst for proton exchange membrane fuel cells

    International Nuclear Information System (INIS)

    Zhu Tong; Du Chunyu; Liu Chuntao; Yin Geping; Shi Pengfei

    2011-01-01

    This paper describes the preparation of SiO 2 stabilized Pt/C catalyst (SiO 2 /Pt/C) by the hydrolysis of alkoxysilane, and examines the possibility that the SiO 2 /Pt/C is used as a durable cathode catalyst for proton exchange membrane fuel cells (PEMFCs). TEM and XRD results revealed that the hydrolysis of alkoxysilane did not significantly change the morphology and crystalline structure of Pt particles. The SiO 2 /Pt/C catalyst exhibited higher durability than the Pt/C one, due to the facts that the silica layers covered were beneficial for reducing the Pt aggregation and dissolution as well as increasing the corrosion resistance of supports, although the benefit of silica covering was lower than the case of Pt/CNT catalyst. Also, it was observed that the activity of the SiO 2 /Pt/C catalyst for the oxygen reduction reaction was somewhat reduced compared to the Pt/C one after the silica covering. This reduction was partially due to the low oxygen kinetics as revealed by the rotating-disk-electrode measurement. Silica covering by hydrolysis of only 3-aminopropyl trimethoxysilane is able to achieve a good balance between the durability and activity, leading to SiO 2 /Pt/C as a promising cathode catalyst for PEMFCs.

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

    Directory of Open Access Journals (Sweden)

    Nur Hidayati

    2016-03-01

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

  5. An anodic alumina supported Ni-Pt bimetallic plate-type catalysts for multi-reforming of methane, kerosene and ethanol

    KAUST Repository

    Zhou, Lu

    2014-05-01

    An anodic alumina supported Ni-Pt bimetallic plate-type catalyst was prepared by a two-step impregnation method. The trace amount 0.08 wt% of Pt doping efficiently suppressed the nickel particle sintering and improved the nickel oxides reducibility. The prepared Ni-Pt catalyst showed excellent performance during steam reforming of methane, kerosene and ethanol under both 3000 h stationary and 500-time daily start-up and shut-down operation modes. Self-activation ability of this catalyst was evidenced, which was considered to be resulted from the hydrogen spillover effect over Ni-Pt alloy. In addition, an integrated combustion-reforming reactor was proposed in this study. However, the sintering of the alumina support is still a critical issue for the industrialization of Ni-Pt catalyst. Copyright © 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

  6. Citric acid induced promoted dispersion of Pt on the support and enhanced catalytic activities for a Pt-based catalyst

    Science.gov (United States)

    Cheng, Tianqiong; Wang, Jianli; Wang, Suning; Cui, Yajuan; Zhang, Hailong; Yan, Shuang; Yuan, Shandong; Chen, Yaoqiang

    2017-12-01

    Citric acid (CA), as the chelating agent, was introduced to obtain the enhanced Pt dispersion and catalytic activities for the Pt-based catalysts supported on oxygen-storage material. The role and content of CA were investigated systematically. It was found that the citric acid-assisted catalysts showed better Pt dispersion and smaller nanoparticle size of Pt. Thus, the catalyst had lower reduction temperature, preferable thermostability and possessed more oxidation state of Pt species under the oxidation atmosphere. The citric acid-induced fresh catalysts were excellent to convert CO and the corresponding aged ones exhibited higher activities for the elimination of all the target pollutants. Among the aged catalysts, P2-a (the mole ratio of Pt/CA is 2:1) presented the best performance. Particularly, compared with the reference sample (Pc-a), the light-off temperatures (T50) of NO, HC and CO for P2-a decreased by 39 °C, 42 °C and 72 °C, respectively, and the full-conversion temperatures (T90) of NO, HC and CO for P2-a decreased by 44 °C, 44 °C and 48 °C, respectively. Therefore, this work provides a facile and valid method to manufacture advanced catalysts for purification of the vehicle exhaust in the future.

  7. An assessment on preparation methods and applications of hydrophobic Pt-catalyst in nuclear and environmental field

    International Nuclear Information System (INIS)

    Ionita, Gh.; Stefanescu, I.; Varlam, Carmen

    2001-01-01

    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 and application of hydrophobic catalysts for use in nuclear and environmental fields. Unlike the conventional hydrophilic catalysts, the hydrophobic catalysts repel the liquid water and allow the transport of the gaseous reactants and reaction products to and from catalytic active centers. For deuterium and tritium separation, over one hundred hydrophobic catalyst types have been prepared in different experimental conditions and by a large diversity of wet proofing methods. The influence of about twenty parameters on catalytic activity have been also studied. The purpose of this paper is: (1) to provide a database for preparation and selection of he most appropriate method for preparing an active hydrophobic catalyst, (2) to show how to use the hydrophobic catalyst and how to operate efficiently the reactor packed with hydrophobic catalyst, (3) to evaluate the performances and potentiality of hydrophobic catalysts in nuclear and environmental field, (4) evaluation of applications of hydrophobic catalysts in nuclear and environmental fields. As result, the following categories are shown: (1) the hydrophobic catalysts based on platinum and Teflon as wet-proofing proved to have the highest activity and the longest stability, (2) the utilization of hydrophobic catalyst as ordered mixed catalytic packing in the trickle bed or separated bed reactors is more efficient and has been entirely proved on industrial scale for tritium separation process, (3) the extension of the applications of hydrophobic catalysts for other processes which take place in the presence of saturated humidity or liquid water in environmental protection field. The merits of hydrophobic Pt-catalysts for tritium separation are discussed in comparison to other

  8. 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)

  9. Effect of Ce on performance and physicochemical properties of Pt-containing automotive emission control catalysts

    International Nuclear Information System (INIS)

    Nunan, J.G.; Silver, R.G.; Bradley, S.A.

    1992-01-01

    Present-day automotive emission control catalysts contain noble metals such as Pt, Pd and Rh all on an alumina support with a variety of promoters. Ce is one of the most important promoters. In this paper, the interaction between Pt and Ce is studied using TPR and STEM on a variety of catalysts. The degree of Pt/Ce interaction is increased by decreasing CeO 2 crystallite size, and to a lesser extent by increasing CeO 2 loading. Direct Pt/Ce interaction leads to a synergistic reduction of both Pt and surface Ce. This reduction qualitatively correlates with catalyst performance after activation in a reducing gas. It is proposed that this synergistic reduction of Pt and Ce is associated with observed improvements in catalyst performance using a non-oscillating exhaust gas

  10. 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.

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

    Science.gov (United States)

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

    2005-12-01

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

  12. Nonalloyed carbon-supported PtRu catalysts for PEMFC applications

    NARCIS (Netherlands)

    Papageorgopoulos, D.C.; De Heer, M.P.; Keijzer, M.; Pieterse, J.A.Z.; de Bruijn, F. A.

    2004-01-01

    PtRu(1:1)/C catalysts were prepared by a process that was claimed previously to lead to non-alloyed Pt and Ru particles, using two different precursors, Ru nitrosyl nitrate and Ru chloride hydrate. Both X-ray diffraction and characterization by cyclic voltammetry point toward Pt and Ru being present

  13. Nonalloyed carbon-supported PtRu catalysts for PEMFC applications

    NARCIS (Netherlands)

    Papageorgopoulos, D.C.; Heer, de M.P.; Keijzer, M.; Pieterse, J.A.Z.; Bruijn, de F.A.

    2004-01-01

    PtRu(1:1)/C catalysts were prepared by a process that was claimed previously to lead to nonalloyed Pt and Ru particles, using twodifferent precursors, Ru nitrosyl nitrate and Ru chloride hydrate. Both X-ray diffraction and characterization by cyclic voltammetrypoint toward Pt and Ru being present as

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

    NARCIS (Netherlands)

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

    2014-01-01

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

  15. 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.

  16. Electrochemical behaviour of PES ionomer and Pt-free catalyst for PEMFCs

    Directory of Open Access Journals (Sweden)

    STEFANIA GIORDANO

    2013-06-01

    Full Text Available Proton Exchange Membrane Fuel Cells (PEMFCs represent promising technologies to the world economy, with many applications and low environmental impact. A most important aspect concerning their widespread implementation is the cost of polymeric membranes, typically perfluorinated membranes and platinum-based catalytic electrode materials, all of which are necessary to promote electrode reactions, thus increasing fuel cell energy efficiency. In this work, we present some data about non-fluorinated polyetheresulphone (PES membranes and Pt-free catalysts, as possible substitutes of the above materials. Their electrochemical behaviour in oxygen reduction reaction in acidic media are investigated and compared with available reference materials.

  17. 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)

  18. 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)

  19. Electrochemical promotion of catalytic reactions with Pt/C (or Pt/Ru/C)//PBI catalysts

    DEFF Research Database (Denmark)

    Petrushina, Irina; Bjerrum, Niels; Bandur, Viktor

    2007-01-01

    The paper is an overview of the results of the investigation on electrochemical promotion of three catalytic reactions: methane oxidation with oxygen, NO reduction with hydrogen at 135 degrees C and Fischer-Tropsch synthesis (FTS) at 170 degrees C in the [CH4/O-2(or NO/H-2 or CO/H-2)/Ar//Pt(or Pt....../Ru)//PBI(H3PO4)/H-2, Ar] fuel cell. It has been shown that the partial methane oxidation to C2H2 and the C-2 selectivity were electrochemically promoted by the negative catalyst polarization. This was also the case in NO reduction with hydrogen for low NO and H-2 partial pressures. In both cases the catalytic...... reactions have been promoted by the electrochemically produced hydrogen. It has been found that the NO reduction with hydrogen on the Pt/PBI strongly depends on NO and hydrogen partial pressures in the working gas mixture. At higher NO and H-2 partial pressures the catalysis is promoted...

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

    Directory of Open Access Journals (Sweden)

    BILJANA M. BABIĆ

    2007-08-01

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

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

    Science.gov (United States)

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

    2008-11-04

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

  2. Proton conductive Pt-Co nanoparticles anchoring on citric acid functionalized graphene for efficient oxygen reduction reaction

    Science.gov (United States)

    Zhao, Yige; Liu, Jingjun; Wu, Yijun; Wang, Feng

    2017-08-01

    Designing highly efficient electro-catalysts for the oxygen reduction reaction (ORR) has been regarded as a demanding task in the development of renewable energy sources. However, little attention has been paid on improving Pt-based catalysts by promoting proton transfer from the electrolyte solutions to the catalyst layer at the cathode. Herein, we design proton conductive Pt-Co alloy nanoparticles anchoring on citric acid functionalized graphene (Pt-Co/CA-G) catalysts for efficient ORR. The facile modification approach for graphene can introduce oxygenated functional groups on the graphene surface to promote proton transfer as well as keeping the high electron conductivity without destroying the graphene original structure. The electrochemical results show that the Pt-Co/CA-G catalyst exhibits more excellent ORR activity and stability than the commercial Pt/C catalyst, which can be attributed to its improved proton transfer ability. The fast proton transfer comes from the hydrogen-bonding networks formed by the interaction between the oxygenated functional groups and water molecules. This work provides not only a novel and simple approach to modify graphene but also an effective strategy to improve Pt-based catalysts for the ORR.

  3. 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)

  4. Pt-based Bi-metallic Monolith Catalysts for Partial Upgrading of Microalgae Oil

    Energy Technology Data Exchange (ETDEWEB)

    Lawal, Adeniyi [Stevens Inst. of Technology, Hoboken, NJ (United States); Manganaro, James [Anasyn LLC, Princeton, NJ (United States); Goodall, Brian [Valicor Renewables LLC, Dexter, MI (United States); Farrauto, Robert [Columbia Univ., New York, NY (United States)

    2015-03-24

    Valicor’s proprietary wet extraction process in conjunction with thermochemical pre-treatment was performed on algal biomass from two different algae strains, Nannochloropsis Salina (N.S.) and Chlorella to produce algae oils. Polar lipids such as phospholipids were hydrolyzed, and metals and metalloids, known catalyst poisons, were separated into the aqueous phase, creating an attractive “pre-refined” oil for hydrodeoxygenation (HDO) upgrading by Stevens. Oil content and oil extraction efficiency of approximately 30 and 90% respectively were achieved. At Stevens, we formulated a Pt-based bi-metallic catalyst which was demonstrated to be effective in the hydro-treating of the algae oils to produce ‘green’ diesel. The bi-metallic catalyst was wash-coated on a monolith, and in conjunction with a high throughput high pressure (pilot plant) reactor system, was used in hydrotreating algae oils from N.S. and Chlorella. Mixtures of these algae oils and refinery light atmospheric gas oil (LAGO) supplied by our petroleum refiner partner, Marathon Petroleum Corporation, were co-processed in the pilot plant reactor system using the Pt-based bi-metallic monolith catalyst. A 26 wt% N.S. algae oil/74 wt % LAGO mixture hydrotreated in the reactor system was subjected to the ASTM D975 Diesel Fuel Specification Test and it met all the important requirements, including a cetane index of 50.5. An elemental oxygen analysis performed by an independent and reputable lab reported an oxygen content of trace to none found. The successful co-processing of a mixture of algae oil and LAGO will enable integration of algae oil as a refinery feedstock which is one of the goals of DOE-BETO. We have presented experimental data that show that our precious metal-based catalysts consume less hydrogen than the conventional hydrotreating catalyst NiMo Precious metal catalysts favor the hydrodecarbonylation/hydrodecarboxylation route of HDO over the dehydration route preferred by base metal

  5. 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.

  6. Seawater splitting for high-efficiency hydrogen evolution by alloyed PtNix electrocatalysts

    Science.gov (United States)

    Zheng, Jingjing

    2017-08-01

    Robust electrocatalyst is a prerequisite to realize high-efficiency hydrogen evolution by water splitting. Expensive platinum (Pt) is a preferred electrode catalyst for state-of-the-art hydrogen evolution reaction (HER). We present here a category of alloyed PtNix electrocatalysts by a facile green chemical reduction method, which are used to catalyze HER during seawater splitting. The catalytic performances are optimized by tuning stoichiometric Pt/Ni ratio, yielding a maximized catalytic behavior for PtNi5 electrode. The minimized onset potential is as low as -0.38 V and the corresponding Tafel slope is 119 mV dec-1. Moreover, the launched alloy electrodes have remarkable stability at -1.2 V over 12 h. The high efficiency as well as good durability demonstrates the PtNix electrocatalysts to be promising in practical applications.

  7. Pt Monolayer Shell on Nitrided Alloy Core—A Path to Highly Stable Oxygen Reduction Catalyst

    Directory of Open Access Journals (Sweden)

    Jue Hu

    2015-07-01

    Full Text Available The inadequate activity and stability of Pt as a cathode catalyst under the severe operation conditions are the critical problems facing the application of the proton exchange membrane fuel cell (PEMFC. Here we report on a novel route to synthesize highly active and stable oxygen reduction catalysts by depositing Pt monolayer on a nitrided alloy core. The prepared PtMLPdNiN/C catalyst retains 89% of the initial electrochemical surface area after 50,000 cycles between potentials 0.6 and 1.0 V. By correlating electron energy-loss spectroscopy and X-ray absorption spectroscopy analyses with electrochemical measurements, we found that the significant improvement of stability of the PtMLPdNiN/C catalyst is caused by nitrogen doping while reducing the total precious metal loading.

  8. Insights on the SO2 Poisoning of Pt3Co/VC and Pt/VC Fuel Cell Catalysts

    Science.gov (United States)

    2010-01-01

    catalyst is performed at the cathode of proton exchange membrane fuel cells ( PEMFCs ) in order to link previously reported results at the elec- trode...stripping voltammetry and underpotential deposition (upd) of copper adatoms. Then the performance of PEMFC cathodes employing 30wt.% Pt3Co/VC and 50wt.% Pt/VC...proton exchange membrane fuel cells( PEMFCs )in order to link previously reported results at the elec- trode/solution interface to the FC environment. First

  9. Synthesis of Ni-Pt catalysts and characterization

    International Nuclear Information System (INIS)

    Santos, Everton R.F. dos; Sousa, Bianca Viana de; Barbosa, Antonielly dos Santos; Leite, Romulo C.N.; Rodrigues, Meiry G.F.

    2009-01-01

    In this work, bifunctionals catalysts using the MCM-22 zeolite as support and the nickel and platinum metal as hydrogenation/dehydrogenation sites were prepared. The method used for metal dispersion on the zeolite was the competitive ion exchange, using the amine complex [Pt(NH 3 ) 4 ]Cl 2 and [Ni(NH 3 ) 6 ]Cl 2 . After the exchange reactions, the samples were calcinated at 500 deg C for 2 hours and reduced at this same temperature under hydrogen flow. The MCM-22 zeolite and samples containing the metal were characterized by the techniques of: EDX, XRD, DTA/TGA. The diffractions of the precursor MCM-22 (P) presented typical peaks of the MWW topology composed by intercalated lamellar layers with organic molecules that are constituents of the template (HMI). According to the XRD pattern of the calcinated sample, no peaks related to the organic material which is responsible to produce the MCM-22 zeolite were detected. By thermogravimetry it was verified that the removal of the template took place between 500 and 650 deg C proving the effectiveness of the removal process. The chemical analysis by X-ray spectrometric was evidenced this the incorporation in the zeolites of platinum and nickel for all the texts in study. Results from XRD confirming the stability and crystal in study of zeolites. (author)

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

    Directory of Open Access Journals (Sweden)

    Lović Jelena D.

    2012-01-01

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

  11. 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....

  12. Enhanced activity and stability of Pt catalysts on functionalized graphene sheets for electrocatalytic oxygen reduction

    Energy Technology Data Exchange (ETDEWEB)

    Kou, Rong; Shao, Yuyan; Wang, Donghai; Engelhard, Mark H.; Kwak, Ja Hun; Wang, Jun; Viswanathan, Vilayanur V.; Wang, Chongmin; Lin, Yuehe; Wang, Yong; Liu, Jun [Pacific Northwest National Laboratory, Richland, WA 99352 (United States); Aksay, Ilhan A. [Department of Chemical Engineering, Princeton University, Princeton, NJ 08544 (United States)

    2009-05-15

    Electrocatalysis of oxygen reduction using Pt nanoparticles supported on functionalized graphene sheets (FGSs) was studied. FGSs were prepared by thermal expansion of graphite oxide. Pt nanoparticles with average diameter of 2 nm were uniformly loaded on FGSs by impregnation methods. Pt-FGS showed a higher electrochemical surface area and oxygen reduction activity with improved stability as compared with the commercial catalyst. Transmission electron microscopy, X-ray photoelectron spectroscopy, and electrochemical characterization suggest that the improved performance of Pt-FGS can be attributed to smaller particle size and less aggregation of Pt nanoparticles on the functionalized graphene sheets. (author)

  13. Ethanol electrooxidation on Pt/C and Pd/C catalysts promoted with oxide

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Changwei [Department of Chemistry and Institute of Nanochemistry, Jinan University, Guangzhou 510632 (China); State Key Laboratory of Optoelectronic Materials and Technologies, School of Physics and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Shen, Pei kang [State Key Laboratory of Optoelectronic Materials and Technologies, School of Physics and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Liu, Yingliang [Department of Chemistry and Institute of Nanochemistry, Jinan University, Guangzhou 510632 (China)

    2007-02-10

    This research aims to investigate Pd-based catalysts as a replacement for Pt-based catalysts for ethanol electrooxidation in alkaline media. The results show that Pd/C has a higher catalytic activity and better steady-state behaviour for ethanol oxidation than that of Pt/C. The effect of the addition of CeO{sub 2} and NiO to the Pt/C and Pd/C electrocatalysts on ethanol oxidation is also studied in alkaline media. The electrocatalysts with a weight ratio of noble metal (Pt, Pd) to CeO{sub 2} of 2:1 and a noble metal to NiO ration 6:1 show the highest catalytic activity for ethanol oxidation. The oxide promoted Pt/C and Pd/C electrocatalysts show a higher activity than the commercial E-TEK PtRu/C electrocatalyst for ethanol oxidation in alkaline media. (author)

  14. Biopolymer-stabilized Pt nanoparticles colloid: a highly active and recyclable catalyst for biphasic catalysis

    International Nuclear Information System (INIS)

    Wang, Yujia; Shen, Yueyue; Qiu, Yunfei; Zhang, Ting; Liao, Yang; Zhao, Shilin; Ma, Jun; Mao, Hui

    2016-01-01

    Noble metal nanoparticles are promising candidates to replace conventional bulk counterparts owing to their high activity and selectivity. To enable catalyst recovery, noble metal nanoparticles are often supported onto solid matrices to prepare heterogeneous catalyst. Although recycle of noble metal nanoparticles is realized by heterogenization, a loss of activity is usually encountered. In the present investigation, Pt nanoparticles with tunable particle size (1.85–2.80 nm) were facilely prepared by using polyphenols as amphiphilic stabilizers. The as-prepared Pt nanoparticles colloid solution could be used as highly active catalyst in aqueous–organic biphasic catalysis. The phenolic hydroxyls of polyphenols could constrain Pt nanoparticles in aqueous phase, and simultaneously, the aromatic scaffold of polyphenols ensured effective interactions between substrates and Pt nanoparticles. As a consequence, the obtained polyphenols-stabilized Pt nanoparticles exhibited high activity and cycling stability in biphasic hydrogenation of a series of unsaturated compounds. Compared with conventional heterogeneous Pt-C and Pt-Al 2 O 3 catalysts, polyphenols-stabilized Pt nanoparticles showed obvious advantage both in activity and cycling stability.

  15. Biopolymer-stabilized Pt nanoparticles colloid: a highly active and recyclable catalyst for biphasic catalysis

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Yujia; Shen, Yueyue; Qiu, Yunfei; Zhang, Ting; Liao, Yang; Zhao, Shilin; Ma, Jun, E-mail: 1044208419@qq.com; Mao, Hui, E-mail: rejoice222@163.com [Sichuan Normal University, College of Chemistry and Materials Science (China)

    2016-10-15

    Noble metal nanoparticles are promising candidates to replace conventional bulk counterparts owing to their high activity and selectivity. To enable catalyst recovery, noble metal nanoparticles are often supported onto solid matrices to prepare heterogeneous catalyst. Although recycle of noble metal nanoparticles is realized by heterogenization, a loss of activity is usually encountered. In the present investigation, Pt nanoparticles with tunable particle size (1.85–2.80 nm) were facilely prepared by using polyphenols as amphiphilic stabilizers. The as-prepared Pt nanoparticles colloid solution could be used as highly active catalyst in aqueous–organic biphasic catalysis. The phenolic hydroxyls of polyphenols could constrain Pt nanoparticles in aqueous phase, and simultaneously, the aromatic scaffold of polyphenols ensured effective interactions between substrates and Pt nanoparticles. As a consequence, the obtained polyphenols-stabilized Pt nanoparticles exhibited high activity and cycling stability in biphasic hydrogenation of a series of unsaturated compounds. Compared with conventional heterogeneous Pt-C and Pt-Al{sub 2}O{sub 3} catalysts, polyphenols-stabilized Pt nanoparticles showed obvious advantage both in activity and cycling stability.

  16. Fuel cell electrocatalsis : oxygen reduction on Pt-based nanoparticle catalysts

    NARCIS (Netherlands)

    Vliet, Dennis Franciscus van der

    2010-01-01

    The thesis contains a discussion on the subject of the Oxygen Reduction Reaction (ORR) on Pt-alloy nanoparticle catalysts in the Rotating Disk Electrode (RDE) method. An insight in some of the difficulties of this method is given with proper solutions and compensations for these problems. Pt3Co,

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

    Science.gov (United States)

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

    2018-05-01

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

  18. Alum an Efficient Catalyst for Erlenmeyer Synthesis

    African Journals Online (AJOL)

    NICO

    this paper we describe the use of alum as a catalyst in the. Erlenmeyer reaction, under solvent-free condition using ultra- sonic irradiation. The application of solvent-free reaction conditions in organic chemistry has been explored extensively within the last decade. It was shown to be an efficient technique for various organic.

  19. SiC nanocrystals as Pt catalyst supports for fuel cell applications

    DEFF Research Database (Denmark)

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

    2013-01-01

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

  20. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-04-15

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

  2. 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...

  3. Preparation of Pt-PTFE hydrophobic catalyst for hydrogen-water isotope exchange

    International Nuclear Information System (INIS)

    Li Junhua; Kang Yi; Han Yande; Ruan Hao; Dou Qincheng; Hu Shilin

    2001-01-01

    The hydrophobic catalyst used in the hydrogen-water isotope exchange is prepared with Pt as the active metal, PTFE as the hydrophobic material, active carbon or silicon dioxide as the support. The isotope catalytic exchange reaction between hydrogen and water is carried out in the trickle bed and the effects of different carriers, mass fraction of Pt and PTFE on the catalytic activity are discussed. The experimental results show that the activity of Pt-C-PTFE hydrophobic catalyst with the ratio between PTFE and Pt-C from 1 to 2 is higher than other kinds of catalysts and the overall volume transfer coefficient is increased with the increasing of the hydrogen flow rate and reaction temperature

  4. 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.

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

    Science.gov (United States)

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

    2017-09-01

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

  6. 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

  7. CO Sensing Performance of a Micro Thermoelectric Gas Sensor with AuPtPd/SnO₂ Catalyst and Effects of a Double Catalyst Structure with Pt/α-Al₂O₃.

    Science.gov (United States)

    Goto, Tomoyo; Itoh, Toshio; Akamatsu, Takafumi; Shin, Woosuck

    2015-12-15

    The CO sensing properties of a micro thermoelectric gas sensor (micro-TGS) with a double AuPtPd/SnO₂ and Pt/α-Al₂O₃ catalyst were investigated. While several nanometer sized Pt and Pd particles were uniformly dispersed on SnO₂, the Au particles were aggregated as particles measuring >10 nm in diameter. In situ diffuse reflectance Fourier transform Infrared spectroscopy (DRIFT) analysis of the catalyst showed a CO adsorption peak on Pt and Pd, but no clear peak corresponding to the interaction between CO and Au was detected. Up to 200 °C, CO combustion was more temperature dependent than that of H₂, while H₂ combustion was activated by repeated exposure to H₂ gas during the periodic gas test. Selective CO sensing of the micro-TGS against H₂ was attempted using a double catalyst structure with 0.3-30 wt% Pt/α-Al₂O₃ as a counterpart combustion catalyst. The sensor output of the micro-TGS decreased with increasing Pt content in the Pt/α-Al₂O₃ catalyst, by cancelling out the combustion heat from the AuPtPd/SnO₂ catalyst. In addition, the AuPtPd/SnO₂ and 0.3 wt% Pt/α-Al₂O₃ double catalyst sensor showed good and selective CO detection. We therefore demonstrated that our micro-TGS with double catalyst structure is useful for controlling the gas selectivity of CO against H₂.

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

    International Nuclear Information System (INIS)

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

    1981-01-01

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

  9. Formic acid decomposition on Pt1/Cu (111) single platinum atom catalyst: Insights from DFT calculations and energetic span model analysis

    Science.gov (United States)

    Wang, Ying-Fan; Li, Kun; Wang, Gui-Chang

    2018-04-01

    Inspired by the recent surface experimental results that the monatomic Pt catalysts has more excellent hydrogen production that Cu(111) surface, the mechanism of decomposition of formic acid on Cu(111) and single atom Pt1/Cu(111) surface was studied by periodic density functional theory calculations in the present work. The results show that the formic acid tends to undergo dehydrogenation on both surfaces to obtain the hydrogen product of the target product, and the selectivity and catalytic activity of Pt1/Cu (111) surface for formic acid dehydrogenation are better. The reason is that the single atom Pt1/Cu(111) catalyst reduces the reaction energy barrier (i.e., HCOO → CO2 + H) of the critical step of the dehydrogenation reaction due to the fact that the single atom Pt1/Cu(111) catalyst binds formate weakly compared to that of Cu (111) one. Moreover, it was found that the Pt1/Cu (111) binds CO more strongly than that of Cu (111) one and thus leading to the difficult for the formation of CO. These two factors would make the single Pt atom catalyst had the high selectivity for the H2 production. It is hoped that the present work may help people to design the efficient H2 production from HCOOH decomposition by reduce the surface binding strength of HCOO species, for example, using the low coordination number active site like single atom or other related catalytic system.

  10. Catalytic activity of hydrophobic Pt/C/PTFE catalysts of different PTFE content for hydrogen-water liquid exchange reaction

    International Nuclear Information System (INIS)

    Hu Sheng; Xiao Chengjian; Zhu Zuliang; Luo Shunzhong; Wang Heyi; Luo Yangming; Wang Changbin

    2007-01-01

    10%Pt/C catalysts were prepared by liquid reduction method. PTFE and Pt/ C catalysts were adhered to porous metal and hydrophobic Pt/C/PTFE catalysts were prepared. The structure and size of Pt crystal particles of Pt/C catalysts were analyzed by XRD, and their mean size was 3.1 nm. The dispersion state of Pt/C and PTFE was analyzed by SEM, and they had good dispersion mostly, but PTFE membrane could be observed on local parts of Pt/C/PTFE surface. Because of low hydrophobicity, Pt/C/ PTFE catalysts have low activity when the mass ratio of PTFE and Pt/C is 0.5: 1, and their catalytic activity increases markedly when the ratio is 1:1. When the ratio increases again, more Pt active sites would be covered by PTFE and interior diffusion effect would increase, which result in the decrease of catalytic activity of Pt/C/PTFE. By PTFE pretreatment of porous metal carrier, the activity of Pt/C/PTFE catalysts decreases when the mass ratio of PTFE and Pt/C is 0.5:1, and their activity decreases when the mass ratio is 1:1. (authors)

  11. 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)

  12. Graphene–poly(5-aminoindole) composite film as Pt catalyst support for methanol electrooxidation in alkaline medium

    International Nuclear Information System (INIS)

    Yue, Ruirui; Zhang, Qiang; Wang, Caiqin; Du, Yukou; Yang, Ping; Xu, Jingkun

    2013-01-01

    Highlights: • Electropolymerization of 5-aminoindole (AIn) in the presence of graphene (GE). • Significant catalytic effect of GE on the polymerization of AIn. • PAIn/GE/GC used as Pt catalyst support. • The enhanced catalytic activity of Pt/PAIn/GE/GC for methanol electrooxidation. -- Abstract: 5-Aminoindole (AIn) was electropolymerized on graphene (GE) modified glass carbon (GC) electrode in 0.5 M H 2 SO 4 aqueous solution containing 0.01 M AIn. Because of the catalytic effect of GE, the polymerization efficiency of AIn and the electrochemical activity of as-formed poly(5-aminoindole) (PAIn) were significantly improved on GE/GC electrode as compared to that on the bare GC electrode. The prepared PAIn/GE/GC electrode was used as substrate for Pt particle electrodeposition. SEM, EDX and Raman spectral were used to characterize the prepared electrodes. Electrocatalytic experiments demonstrate that the Pt/PAIn/GE/GC electrode possesses high catalytic activity toward methanol electrooxidation in alkaline medium, due to the good dispersion of Pt particles on PAIn/GE/GC and the electronic interactions between the metal particles and the polymer matrixes. Thus, PAIn can be a promising alternative for polymeric catalyst support in direct alcohol fuel cells

  13. Synthesis and characterization of PtRu/C catalysts obtained by colloidal and deposition methods for fuel cell applications

    Directory of Open Access Journals (Sweden)

    Egberto Gomes Franco

    2005-06-01

    Full Text Available The purpose of this investigation was to compare catalysts produced by the Bönnemann - colloidal method (PtRu (B1 and PtRu (B2, and those produced by the spontaneous deposition method (PtRu (SD. The catalysts produced by both methods had good electrochemical behavior for methanol oxidation for proton exchange membrane fuel cell applications. The structure of the catalyst was examined by transmission electron microscopy (TEM. Energy dispersive spectroscopic analysis (EDS was used to determine the semi-quantitative composition of the catalysts, and the electrochemical behavior was determined by cyclic voltammetry (CV. The diffractograms of the binary catalysts revealed platinum and ruthenium as the only crystalline phases, as per ICDD data base. The PtRu (B1 catalyst, treated in a reducing atmosphere, has the same structure as PtRu (B2, treated in an oxidising/reducing atmosphere, except that the crystallite size was around 1.7 nm for PtRu (B1 instead of 9.9 nm for PtRu (B2. The catalysts PtRu (B2 and PtRu (SD showed similar cyclic voltammetric behavior, which was better than that of PtRu (B1. Both methods are suitable for the production of electrocatalysts for fuel cell applications. The colloidal method is more expensive than the deposition method, but the former permits the production of ternary and quaternary catalyst systems with enhanced CO tolerance.

  14. 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.

  15. Catalysts for Efficient Production of Carbon Nanotubes

    Science.gov (United States)

    Sun, Ted X.; Dong, Yi

    2009-01-01

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

  16. Mechanistic Investigation of the Reduction of NOx over Pt- and Rh-Based LNT Catalysts

    Directory of Open Access Journals (Sweden)

    Lukasz Kubiak

    2016-03-01

    Full Text Available The influence of the noble metals (Pt vs. Rh on the NOx storage reduction performances of lean NOx trap catalysts is here investigated by transient micro-reactor flow experiments. The study indicates a different behavior during the storage in that the Rh-based catalyst showed higher storage capacity at high temperature as compared to the Pt-containing sample, while the opposite is seen at low temperatures. It is suggested that the higher storage capacity of the Rh-containing sample at high temperature is related to the higher dispersion of Rh as compared to Pt, while the lower storage capacity of Rh-Ba/Al2O3 at low temperature is related to its poor oxidizing properties. The noble metals also affect the catalyst behavior upon reduction of the stored NOx, by decreasing the threshold temperature for the reduction of the stored NOx. The Pt-based catalyst promotes the reduction of the adsorbed NOx at lower temperatures if compared to the Rh-containing sample, due to its superior reducibility. However, Rh-based material shows higher reactivity in the NH3 decomposition significantly enhancing N2 selectivity. Moreover, formation of small amounts of N2O is observed on both Pt- and Rh-based catalyst samples only during the reduction of highly reactive NOx stored at 150 °C, where NOx is likely in the form of nitrites.

  17. Characterization of Pt catalysts supported in mixed oxides

    International Nuclear Information System (INIS)

    Perez H, R.; Garcia C, M.A.; Gomez C, A.; Diaz, G.

    1999-01-01

    The catalytic supports TiO 2 , ZrO 2 and TiO 2 -ZrO 2 were prepared by the sol-gel technique. The incorporation of Pt to the supports was by the classical impregnation method. The catalytic materials were characterized (Pt/TiO 2 , Pt/ZrO 2 and Pt/TiO 2 -ZrO 2 ) by diverse techniques to determine: the texture (BET), evolution of the catalytic materials synthesised after drying and calcination (Infrared spectroscopy) and by Thermogravimetric analysis. (Author)

  18. Experimental and DFT study of thiol-stabilized Pt/CNTs catalysts.

    Science.gov (United States)

    Li, L; Chen, S G; Wei, Z D; Qi, X Q; Xia, M R; Wang, Y Q

    2012-12-28

    Using a combination of experiments and density functional theory (DFT) calculations, we explored the mechanisms of the stabilization effect of the thiolized (-SH) group on the Pt/SH-CNTs catalyst. Pt particles supported on the hydroxyl functionalized CNTs (Pt/OH-CNTs) are synthesized as a baseline for comparison. Experimentally, the platinum on OH-CNTs has a stronger tendency for aggregation than that on SH-CNTs. The differences in the oxidation resistance, migration activation energy, and corrosion resistance between the Pt/SH-CNTs and Pt/OH-CNTs are calculated using DFT. The DFT calculations indicate that the -SH group enhances the oxidation resistance of the Pt cluster and CNTs and restricts Pt migration on the CNTs. DFT calculations also suggest that the enhanced stability of Pt/SH-CNTs originates from the increased interaction between Pt and SH-CNTs and the depressed d-band center of the Pt NPs. Thus, the functional groups on the CNTs used for stabilization of supported Pt NPs should provide a deposit and anchor site for Pt NPs and maintain the perfect structure of CNTs rather than destroying it.

  19. Effects of K and Pt promoters on the performance of cobalt catalyst supported on CNTs

    International Nuclear Information System (INIS)

    Zabidi, Noor Asmawati Mohd; Ali, Sardar; Subbarao, Duvvuri

    2014-01-01

    This paper presents a comparative study on the effects of incorporation of potassium (K) and platinum (Pt) as promoters on the physicochemical properties of cobalt catalyst. The catalyst was prepared by a wet impregnation method on a CNTs support. Samples were characterized using transmission electron microscopy (TEM), H 2 -temperature-programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS) techniques. Fischer-Tropsch Synthesis (FTS) was carried out in a fixed-bed microreactor at 543 K and 1 atm, with H 2 /CO = 2v/v and space velocity, SV of 12 L/g.h for 5 hours. The K-promoted and Pt-promoted Co catalysts have different physicochemical properties and catalytic performances compared to that of the un-promoted Co catalyst. XPS analysis revealed that K and Pt promoters induced electronic modifications as exhibited by the shifts in the Co binding energies. Incorporation of 0.06 wt% K and 0.06 wt% Pt in Co/CNTs catalyst resulted in an increase in the CO conversion and C 5+ selectivity and a decrease in methane selectivity. Potassium was found to be a better promoter for Co/CNTs catalyst compared to platinum

  20. Effects of K and Pt promoters on the performance of cobalt catalyst supported on CNTs

    Energy Technology Data Exchange (ETDEWEB)

    Zabidi, Noor Asmawati Mohd, E-mail: noorasmawati-mzabidi@petronas.com.my [Department of Fundamental and Applied Sciences, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak (Malaysia); Ali, Sardar, E-mail: alikhan-635@yahoo.com [Centralized Analytical Laboratory, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak (Malaysia); Subbarao, Duvvuri, E-mail: duvvuri-subbarao@petronas.com.my [Department of Chemical Engineering, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750 Tronoh, Perak (Malaysia)

    2014-10-24

    This paper presents a comparative study on the effects of incorporation of potassium (K) and platinum (Pt) as promoters on the physicochemical properties of cobalt catalyst. The catalyst was prepared by a wet impregnation method on a CNTs support. Samples were characterized using transmission electron microscopy (TEM), H{sub 2}-temperature-programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS) techniques. Fischer-Tropsch Synthesis (FTS) was carried out in a fixed-bed microreactor at 543 K and 1 atm, with H{sub 2}/CO = 2v/v and space velocity, SV of 12 L/g.h for 5 hours. The K-promoted and Pt-promoted Co catalysts have different physicochemical properties and catalytic performances compared to that of the un-promoted Co catalyst. XPS analysis revealed that K and Pt promoters induced electronic modifications as exhibited by the shifts in the Co binding energies. Incorporation of 0.06 wt% K and 0.06 wt% Pt in Co/CNTs catalyst resulted in an increase in the CO conversion and C{sub 5+} selectivity and a decrease in methane selectivity. Potassium was found to be a better promoter for Co/CNTs catalyst compared to platinum.

  1. Effects of composition on structure and activity of PtRu/C catalysts.

    Science.gov (United States)

    Wiltshire, Richard J K; King, Colin R; Rose, Abigail; Wells, Peter P; Davies, Hazel; Hogarth, Martin P; Thompsett, David; Theobald, Brian; Mosselmans, Fredrick W; Roberts, Mark; Russell, Andrea E

    2009-04-07

    A series of carbon supported PtRu bimetallic catalysts with varying Pt:Ru ratio were prepared and characterised using ex situ and in situ XRD, in situ EXAFS at 0 V vs. RHE, ex situ XPS and monolayer CO stripping voltammetry. Although the catalysts were found to be well mixed/alloyed, with no evidence of unalloyed Ru (oxides) present, the surfaces of the electrocatalyst nanoparticles were found to be enriched with Pt compared to the nominal bulk composition. The methanol oxidation activities of the catalysts were determined in 1.0 mol dm(-3) H2SO4. In agreement with published studies of polycrystalline bulk PtRu alloys the catalyst with a 0.6 surface fraction of Pt was found to give the best methanol oxidation activity at 30 degrees C. However, at 80 degrees C a greater surface fraction of Ru could be tolerated, with some activity at low current densities found for a Pt surface fraction as low as 0.2. The results support the conclusion that a limited amount of methanol dehydrogenation occurs at Ru sites or Ru dominated surface ensembles at 80 degrees C.

  2. One-pot synthesis of reduced graphene oxide supported PtCuy catalysts with enhanced electro-catalytic activity for the methanol oxidation reaction

    International Nuclear Information System (INIS)

    Peng, Xinglan; Zhao, Yanchun; Chen, Duhong; Fan, Yanfang; Wang, Xiao; Wang, Weili; Tian, Jianniao

    2014-01-01

    The outstanding performance PtCu y (y = 1,2,3) alloy nanoparticles supported on reduced graphene oxide (rGO) have been synthesized by a facile, efficient, one-pot hydrothermal synthesis approach. The as-prepared PtCu y /rGO catalysts are comprehensively characterized by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy. Cyclic voltammetry, CO-stripping voltammetry and chronoamperometry results reveal that the PtCu y /rGO catalysts have higher electro-catalytic activity, more negative onset oxidative potential, more excellent tolerance ability for CO poisoning and enhanced stability for the electro-oxidation of methanol compared to pure Pt/rGO. As far as the as-made PtCu y /rGO catalysts are concerned, the PtCu 2 /rGO exhibits the highest electro-catalytic activity. The mechanism of the promoting effect of Cu on Pt is explained based on the electronic modification effect. The nature of interfacial interactions between the Pt-Cu active metal phase and the rGO supporting materials is crucial to achieving high performance

  3. Spectroelectrochemical Study of Carbon Monoxide and Ethanol Oxidation on Pt/C, PtSn(3:1/C and PtSn(1:1/C Catalysts

    Directory of Open Access Journals (Sweden)

    Rubén Rizo

    2016-09-01

    Full Text Available PtSn-based catalysts are one of the most active materials toward that contribute ethanol oxidation reaction (EOR. In order to gain a better understanding of the Sn influence on the carbon monoxide (principal catalyst poison and ethanol oxidation reactions in acidic media, a systematic spectroelectrochemical study was carried out. With this end, carbon-supported PtSnx (x = 0, 1/3 and 1 materials were synthesized and employed as anodic catalysts for both reactions. In situ Fourier transform infrared spectroscopy (FTIRS and differential electrochemical mass spectrometry (DEMS indicate that Sn diminishes the amount of bridge bonded CO (COB and greatly improves the CO tolerance of Pt-based catalysts. Regarding the effect of Sn loading on the EOR, it enhances the catalytic activity and decreases the onset potential. FTIRS and DEMS analysis indicate that the C-C bond scission occurs at low overpotentials and at the same potential values regardless of the Sn loading, although the amount of C-C bond breaking decreases with the rise of Sn in the catalytic material. Therefore, the elevated catalytic activity toward the EOR at PtSn-based electrodes is mainly associated with the improved CO tolerance and the incomplete oxidation of ethanol to form acetic acid and acetaldehyde species, causing the formation of a higher amount of both C2 products with the rise of Sn loading.

  4. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-01-10

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

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

    International Nuclear Information System (INIS)

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

    2008-01-01

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

  7. CO oxidation on PtSn nanoparticle catalysts occurs at the interface of Pt and Sn oxide domains formed under reaction conditions

    KAUST Repository

    Michalak, William D.; Krier, James M.; Alayoglu, Selim; Shin, Jae-Yoon; An, Kwangjin; Komvopoulos, Kyriakos; Liu, Zhi; Somorjai, Gabor A.

    2014-01-01

    The barrier to CO oxidation on Pt catalysts is the strongly bound adsorbed CO, which inhibits O2 adsorption and hinders CO2 formation. Using reaction studies and in situ X-ray spectroscopy with colloidally prepared, monodisperse ∼2 nm Pt and PtSn

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

    Directory of Open Access Journals (Sweden)

    S. STEVANOVIC

    2008-08-01

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

  9. 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

  10. Low Pt content direct methanol fuel cell anode catalyst: nanophase PtRuNiZr

    Science.gov (United States)

    Narayanan, Sekharipuram R. (Inventor); Whitacre, Jay F. (Inventor)

    2010-01-01

    A method for the preparation of a metallic material having catalytic activity that includes synthesizing a material composition comprising a metal content with a lower Pt content than a binary alloy containing Pt but that displays at least a comparable catalytic activity on a per mole Pt basis as the binary alloy containing Pt; and evaluating a representative sample of the material composition to ensure that the material composition displays a property of at least a comparable catalytic activity on a per mole Pt basis as a representative binary alloy containing Pt. Furthermore, metallic compositions are disclosed that possess substantial resistance to corrosive acids.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-10-15

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

  12. High-temperature electrochemical characterization of Ru core Pt shell fuel cell catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Bokach, D.; Fuente, J.L.G. de la; Tsypkin, M.; Ochal, P.; Tunold, R.; Sunde, S.; Seland, F. [Department of Materials Science and Engineering, Norwegian University of Science and Technology (NTNU), Sem Saelands veg 12, N-7491 Trondheim (Norway); Endsjoe, I.C. [Washington Mills AS, NO-7300 Orkanger (Norway)

    2011-12-15

    The electrooxidation of methanol was studied at elevated temperature and pressure by cyclic voltammetry and constant potential experiments at real fuel cell electrocatalysts. Ruthenium core and platinum shell nanoparticles were synthesized by a sequential polyol route, and characterized electrochemically by CO stripping at room temperature to quickly confirm the structure of the synthesized core-shell structure as compared to pure commercial Pt/C and Pt-Ru/C alloy catalysts. A significant promotional effect of Pt decorated Ru cores in the methanol oxidation was found at elevated temperatures and rather high-electrode potentials. A negative potential shift of the methanol oxidation peak is observed for the Ru rate at Pt/C core-shell catalyst at moderate temperatures, while a significant shift to positive potentials of the methanol oxidation peak occurs for Pt/C catalysts. The onset potential for methanol oxidation is lowered some 200 mV from room temperature and up to 120 C for all electrocatalysts, indicating that it is the thermal activity of water adsorption that dictates the onset potential. Direct methanol fuel cell experiments showed only small performance differences between Ru rate at Pt/C and Pt/C anode electrocatalysts, suggesting the necessity of render possible the formation of surface oxygen species at lower electrode potentials. (Copyright copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  13. One-pot catalytic conversion of cellulose into polyols with Pt/CNTs catalysts.

    Science.gov (United States)

    Yang, Li; Yan, Xiaopei; Wang, Qiwu; Wang, Qiong; Xia, Haian

    2015-03-02

    A series of Pt nanoparticles supported on carbon nanotubes (CNTs) were synthesized using the incipient-wetness impregnation method. These catalysts were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), Raman spectroscopy, and transmission electron microscope (TEM) techniques. The characterization results indicate that the Pt nanoparticles were highly dispersed on the surface of the CNTs, and the mean size was less than 5 nm. These catalysts were utilized to convert cellulose to hexitol, ethylene glycerol (EG), and 1,2-propylene glycol (1,2-PG) under low H2 pressure. The total yields were as high as 71.4% for EG and 1,2-PG using 1Pt/CNTs as the catalyst in the hydrolytic hydrogenation of cellulose under mild reaction conditions. Copyright © 2014 Elsevier Ltd. All rights reserved.

  14. Synthesis and Immobilization of Pt Nanoparticles on Amino-Functionalized Halloysite Nanotubes toward Highly Active Catalysts

    Directory of Open Access Journals (Sweden)

    Tingting Yang

    2015-02-01

    Full Text Available A simple and effective method for the preparation of platinum nanoparticles (Pt NPs grown on amino-func‐ tionalized halloysite nanotubes (HNTs was developed. The nanostructures were synthesized through the func‐ tionalization of the HNTs, followed by an in situ approach to generate Pt NPs with diameter of approximately 1.5 nm within the entire HNTs. The synthesis process, composition and morphology of the nanostructures were characterized. The results suggest PtNPs/NH2-HNTs nanostructures with ultrafine PtNPs were successfully synthesized by green chemically-reducing H2PtCl6 without the use of surfactant. The nanostructures exhibit promising catalytic properties for reducing potassium hexacyanoferrate(III to potassium hexacyanoferrate(II. The presented experiment for novel PtNPs/NH2-HNTs nanostructures is quite simple and environmentally benign, permitting it as a potential application in the future field of catalysts.

  15. Effect of TiB2 Pretreatment on Pt/TiB2 Catalyst Performance

    International Nuclear Information System (INIS)

    Huang, Zhen; Lin, Rui; Fan, Renjie; Fan, Qinbai; Ma, Jianxin

    2014-01-01

    Highlights: • We pretreated Titanium diboride by different acids and alkali. • We synthesis the Pt/as-pretreated TiB 2 catalysts by a colloid route. • We investigated the effects of TiB 2 Pretreatment on Pt/TiB 2 Catalyst Performance. • The BET surface area and defects on the surface have a close relationship with the deposition of Pt nanoparticles. - Abstract: Carbon support corrosion of traditional Pt/C catalyst is one of the major contributors causing poor durability of proton exchange membrane fuel cells (PEMFC). Titanium diboride (TiB 2 ) has high electrical conductivity and considerable chemical stability, which making it as a good candidate for catalyst support in PEMFC. In this work, TiB 2 was pretreated by different acid and alkali. The as-obtained samples were characterized by Ex-situ microscopy (ESM) and X-ray diffraction (XRD). The pore size distribution (PSD) was analyzed by using DFT method. The PSD shows distinct volume in mesopore regions (less than 50 nm). The TiB2 pretreated by H 2 O 2 shows the biggest BET surface area of 57 m 2 g −1 and its PSD focus on mesoporous (1.5-8 nm) region, which resulted to high dispersion and better loading of Pt particles. The Hydrogen oxidization reaction (HOR) and oxygen reduction reaction (ORR) activity was characterized by Rotating Disk Electrode (RDE). The Pt/TiB 2 prepared by H 2 O 2 -pretreated TiB 2 using the colloidal method showed better half-cell electrochemical performance. Facile synthetic for the development of Pt/TiB 2 catalysts was developed

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

    Science.gov (United States)

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

    2014-03-24

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

  17. Further studies on hydration of alkynes by the PtCl4-CO catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Israelsohn, Osnat; Vollhardt, K. Peter C.; Blum, Jochanan

    2002-01-18

    Under CO atmosphere, between 80 and 120 C, a glyme solution of PtCl{sub 4} forms a carbonyl compound that promotes hydration of internal as well as terminal alkynes to give aldehyde-free ketones. The catalytic process depends strongly on the electronic and steric nature of the substrates. Part of the carbonyl functions of the catalyst can be replaced by phosphine ligands. Chiral DIOP reacts with the PtCl{sub 4}-CO compound to give a catalyst that promotes partial kinetic resolution of a racemic alkyne. Replacement of part of the CO by polystyrene-bound diphenylphosphine enables to attach the catalyst to the polymeric support. Upon entrapment of the platinum compound in a silica sol-gel matrix, it reacts as a partially recyclable catalyst. A reformulated mechanism for the PdCl{sub 4}-CO catalyzed hydration is suggested on the basis of the present study.

  18. Pt Catalyst Supported within TiO2 Mesoporous Films for Oxygen Reduction Reaction

    International Nuclear Information System (INIS)

    Huang, Dekang; Zhang, Bingyan; Bai, Jie; Zhang, Yibo; Wittstock, Gunther; Wang, Mingkui; Shen, Yan

    2014-01-01

    In this study, dispersed Pt nanoparticles into mesoporous TiO 2 thin films are fabricated by a facile electrochemical deposition method as electro-catalysts for oxygen reduction reaction. The mesoporous TiO 2 thin films coated on the fluorine-doped tin oxide glass by screen printing allow a facile transport of reactants and products. The structural properties of the resulted Pt/TiO 2 electrode are evaluated by field emission scanning electron microscopy, energy dispersive X-ray spectrometry, X-ray diffraction, and X-ray photoelectron spectroscopy. Cyclic voltammetry measurements are performed to study the electrochemical properties of the Pt/TiO 2 electrode. Further study demonstrates the stability of the Pt catalyst supported within TiO 2 mesoporous films for the oxygen reduction reaction

  19. Effect of Particle Size and Operating Conditions on Pt3Co PEMFC Cathode Catalyst Durability

    Directory of Open Access Journals (Sweden)

    Mallika Gummalla

    2015-05-01

    Full Text Available The initial performance and decay trends of polymer electrolyte membrane fuel cells (PEMFC cathodes with Pt3Co catalysts of three mean particle sizes (4.9 nm, 8.1 nm, and 14.8 nm with identical Pt loadings are compared. Even though the cathode based on 4.9 nm catalyst exhibited the highest initial electrochemical surface area (ECA and mass activity, the cathode based on 8.1 nm catalyst showed better initial performance at high currents. Owing to the low mass activity of the large particles, the initial performance of the 14.8 nm Pt3Co-based electrode was the lowest. The performance decay rate of the electrodes with the smallest Pt3Co particle size was the highest and that of the largest Pt3Co particle size was lowest. Interestingly, with increasing number of decay cycles (0.6 to 1.0 V, 50 mV/s, the relative improvement in performance of the cathode based on 8.1 nm Pt3Co over the 4.9 nm Pt3Co increased, owing to better stability of the 8.1 nm catalyst. The electron microprobe analysis (EMPA of the decayed membrane-electrode assembly (MEA showed that the amount of Co in the membrane was lower for the larger particles, and the platinum loss into the membrane also decreased with increasing particle size. This suggests that the higher initial performance at high currents with 8.1 nm Pt3Co could be due to lower contamination of the ionomer in the electrode. Furthermore, lower loss of Co from the catalyst with increased particle size could be one of the factors contributing to the stability of ECA and mass activity of electrodes with larger cathode catalyst particles. To delineate the impact of particle size and alloy effects, these results are compared with prior work from our research group on size effects of pure platinum catalysts. The impact of PEMFC operating conditions, including upper potential, relative humidity, and temperature on the alloy catalyst decay trends, along with the EMPA analysis of the decayed MEAs, are reported.

  20. Hydroisomerization of n-dodecane over Pt/Al-MCM-48 catalysts.

    Science.gov (United States)

    Yun, Soyoung; Park, Young-Kwon; Jeong, Soon-Yong; Han, Jeongsik; Jeon, Jong-Ki

    2014-04-01

    The objective of this study is to evaluate the catalytic potential of Pt/Al-MCM-48 catalysts in hydroisomerization of n-dodecane. The effects of the Si/Al ratio and platinum loading on the acid characteristics of Al-MCM-48 and the catalytic performance in n-dodecane hydroisomerization were analyzed. The catalysts were characterized by X-ray diffraction, nitrogen adsorption, infrared spectroscopy of pyridine adsorption, and temperature programmed desorption of ammonia. The number of weak strength acid sites on Al-MCM-48 increased with 0.5 wt% platinum loading. The weak strength acid sites of Pt/Al-MCM-48 catalysts were ascribed to Lewis acid sites, which can be confirmed by NH3-TPD and FTIR spectra of pyridine adsorption. Iso-dodecane can be produced with high selectivity in n-dodecane hydrosisomerization over Pt/Al-MCM-48 catalysts. This is attributed to the mild acidic properties of Pt/Al-MCM-48 catalysts.

  1. ETEM observation of Pt/C electrode catalysts in a moisturized cathode atmosphere

    International Nuclear Information System (INIS)

    Yoshida, K; Zhang, X; Tanaka, N; Boyes, E D; Gai, P L

    2014-01-01

    There have been reports of challenges in designing platinum carbon (Pt/C) electrode catalysts for PEMFC. Pt/C electrode catalysts deactivate much faster on the cathode (in moisturized O 2 ) than on the anode (in H 2 ). To understand influences of moisture and oxygen on the deactivation of the Pt/C catalysts in proton-exchange-membrane fuel cells (PEMFCs), spherical-aberration-corrected environmental transmission electron microscopy (AC-ETEM) was applied with a high-speed CCD camera. Structural changes of the Pt/C electrode catalysts were dynamically recorded in moisturized nitrogen, oxygen and hydrogen. The mass spectrometry confirmed the moisture content (between 5 to 30 %) of nitrogen driving gas through a humidifier. Coalescence of platinum nanoparticles (D = 3.24 nm) was carefully evaluated in pure N 2 and moisturized N 2 atmosphere. The Pt/C showed considerable structural weakness in a moisturized N2 atmosphere. Comparable results obtained by AC-ETEM in different gas atmospheres also suggested ways to improve the oxygen reduction reaction (ORR). In this paper, the deactivation process due to moisture (hydroxylation) of carbon supports is discussed using for comparison the movement of platinum nanoparticles measured in moisturized nitrogen and pure nitrogen atmospheres

  2. The influence of boron dopant on the electrochemical properties of graphene as an electrode material and a support for Pt catalysts

    International Nuclear Information System (INIS)

    Bo, Xiangjie; Li, Mian; Han, Ce; Guo, Liping

    2013-01-01

    Highlights: •More defective sites in graphene after the doping of boron atoms. •Fine dispersion of Pt nanoparticles supported on boron-doped graphene. •Low electron transfer resistance at boron-doped graphene. •High performance of boron-doped graphene as an electrode material or a support for Pt catalysts. -- Abstract: Boron-doped graphene (BGR) is prepared by thermal annealing of graphene oxide (GO) in the presence of boric acid. More defective sites are introduced into GR accompanied by the doping of boron. Low electron transfer resistance towards redox probe is observed at BGR. The BGR modified electrode can effectively distinguish the anodic peaks for ascorbic acid (AA), dopamine (DA), and uric acid (UA). The defective sites of BGR can also act as anchoring sites for the deposition of Pt nanoparticles. When used as a support for Pt electrocatalysts, Pt nanoparticles with an average diameter of 3.2 nm are deposited on BGR. The doping of boron into GR facilitates the dispersion of Pt nanoparticles and increases the utilization efficiency of Pt nanoparticles. The Pt/BGR exhibits significant catalytic activity towards the oxidation of methanol. The results demonstrate that BGR is a good support for Pt catalysts or an electrode material compared with the undoped GR

  3. Pt Combustion Catalysts Prepared from W/O Microemulsions

    Czech Academy of Sciences Publication Activity Database

    Rymeš, Jan; Ehret, G.; Hilaire, L.; Jirátová, Květa

    2002-01-01

    Roč. 143, - (2002), s. 121-129 ISSN 0167-2991. [International Symposium Scientific Bases for the Preparation of Heterogeneous Catalysts /8./. Louvain-la-Neuve, 09.09.2002-12.09.2002] R&D Projects: GA AV ČR IAA4072904 Keywords : combustion catalysts * microemulsion s Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 3.468, year: 2002

  4. Re-examination of the Pt Particle Size Effect on the Oxygen Reduction Reaction for Ultrathin Uniform Pt/C Catalyst Layers without Influence from Nafion

    International Nuclear Information System (INIS)

    Shinozaki, Kazuma; Morimoto, Yu; Pivovar, Bryan S.; Kocha, Shyam S.

    2016-01-01

    Highlights: • Pt particle size effect on ORR was re-evaluated for Pt/C catalysts. • Nafion-free activity of Pt/C catalysts was evaluated using thin-film RDE methods. • Ultrathin-uniform catalyst layers were employed to obtain accurate activity values. • Specific activity increased steeply from 2 to 10 nm and less steeply at over 10 nm. • Re-evaluated effect agrees with a particle model assuming terrace active sites. - Abstract: The platinum ‘particle size effect’ on the oxygen reduction reaction (ORR) has been re-evaluated using commercial Pt/C catalysts (2–10 nm Pt particle) and polycrystalline Pt (poly-Pt) in 0.1 M HClO 4 with a rotating disk electrode method. Nafion-free catalyst layers were employed to obtain specific activities (SA) that were not perturbed (suppressed) by sulfonate anion adsorption/blocking. By using ultrathin uniform catalyst layers, O 2 diffusion limitation was minimized as confirmed from the high SAs of our supported catalysts that were comparable to unsupported sputtered Pt having controlled sizes. The specific activity (SA) steeply increased for the particle sizes in the range ∼2–10 nm (0.8–1.8 mA/cm 2 Pt at 0.9 V vs. RHE) and plateaued over ∼10 nm to 2.7 mA/cm 2 Pt for bulk poly-Pt. On the basis of the activity trend for the range of particle sizes studied, it appears that the effect of carbon support on activity is negligible. The experimental results and the concomitant profile of SA vs. particle size was found to be in an agreement to a truncated octahedral particle model that assumes active terrace sites.

  5. Insight into the Effect of Sn on CO and Formic Acid Oxidation at PtSn Catalysts

    DEFF Research Database (Denmark)

    Stevanović, S.; Tripković, D.; Tripkovic, Vladimir

    2014-01-01

    The role of Sn on the catalytic activity for CO and formic acid oxidation is studied by comparing the activities of differently treated PtSn/C and Pt/C catalysts. The catalysts are prepared by a microwave-assisted polyol synthesis method. As revealed by scanning tunneling and transmission electron...

  6. 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...

  7. Synthesis of Pt/rGO catalysts with two different reducing agents and their methanol electrooxidation activity

    Energy Technology Data Exchange (ETDEWEB)

    Vu, Thu Ha Thi, E-mail: ptntd2004@yahoo.fr [Key Laboratory for Petrochemical and Refinery Technologies, 2 Pham Ngu Lao street, Hanoi (Viet Nam); Tran, Thanh Thuy Thi, E-mail: tranthithanhthuygl@gmail.com [Key Laboratory for Petrochemical and Refinery Technologies, 2 Pham Ngu Lao street, Hanoi (Viet Nam); Le, Hong Ngan Thi; Tran, Lien Thi; Nguyen, Phuong Hoa Thi; Nguyen, Minh Dang [Key Laboratory for Petrochemical and Refinery Technologies, 2 Pham Ngu Lao street, Hanoi (Viet Nam); Quynh, Bui Ngoc [Institut de recherches sur la catalyse et l’environnement de Lyon, UMR5256, 2 avenue Albert Einstein, 69626 Villeurbanne cedex (France)

    2016-01-15

    Highlights: • Pt/rGO catalysts were successfully synthesized using either NaBH{sub 4} or ethylene glycol. • Synthesis using NaBH{sub 4} could improve electrocatalytic towards methanol oxidation of Pt/rGO catalyst. • 40%Pt/rGO synthesized using NaBH{sub 4} showed the best electrocatalytic performance. - Abstract: The synthesis processes of Platinum (Pt) on reduced graphene oxide (rGO) catalysts from graphene oxide (GO) using two reducing agents including sodium borohydride and ethylene glycol is reported. Structure and morphology of Pt/rGO catalysts are characterized by X-ray powder diffraction, transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. Electrocatalytic methanol oxidation properties of these catalysts are evaluated by cyclic voltammetry and chronoamperometry. The results show that catalyst synthesized using sodium borohydride has a higher metallic Pt content and an improved catalytic performance in comparison to catalyst synthesized using ethylene glycol. Moreover, effect of Pt loading amount on electrocatalytic methanol oxidation performance of catalysts synthesized using sodium borohydride is systematically investigated. The optimal Pt loading amount on graphene is determined to be 40%.

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

    Science.gov (United States)

    Jung, Won Suk; Popov, Branko N

    2017-07-19

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

  9. Effect of W on activity of Pt-Ru/C catalyst for methanol electrooxidation in acidic medium

    International Nuclear Information System (INIS)

    Wang Zhenbo; Zuo Pengjian; Yin Geping

    2009-01-01

    The effect of W on the activity of Pt-Ru/C catalyst was investigated. The Pt-Ru-W/C and Pt-Ru/C-TR catalysts were prepared by thermal reduction method. Comparison was made to a homemade Pt-Ru/C-CR catalyst prepared by chemical reduction. Their performances were tested by using a glassy carbon thin film electrode through cyclic voltammetric and chronoamperometric curves. The particle size, structure, composition, and surface state of homemade catalyst were determined by means of X-ray diffraction (XRD), energy dispersive analysis of X-ray (EDAX), transmission electron microscopy (TEM), and X-ray photoelectron spectrometry (XPS). The result of XRD analysis shows that the homemade ternary catalyst exhibits face-centered cubic structure and has smaller lattice parameter than Pt-alone and homemade Pt-Ru/C catalysts. The particle size of Pt-Ru-W/C catalyst is relatively large of 6.5 nm. Its electrochemically active specific area is 20 m 2 g -1 less than that of Pt-Ru/C-CR, and much twice as big as that of Pt-Ru/C-TR. But, XPS analysis shows that the addition of W changes the surface state of Pt components in the alloy and can clean Pt surface active sites which are adsorbed by hydrogen. The electrocatalytic activity and tolerance performance to CO ads of Pt-Ru-W/C catalyst for methanol electrooxidation is the best due to the promoting function of W in comparison with homemade Pt-Ru/C ones.

  10. Influence of ceria on the thermally durability of Pt/Rh automotive catalyst

    International Nuclear Information System (INIS)

    Muraki, H.; Zhang, G.

    1998-01-01

    Full text: The use of cerium oxide as an oxygen storage component in automotive three-way catalysts has been well established. More recently the requirement of the three-way catalysts against the increase of the severity in emission standards has focused attention on the development of more active, durable catalysts. The thermally durability of Pt/Rh catalyst can be achieved by the utilization of thermally stable ceria as well as optimization of washcoat composition and structure in order to control the extent of interaction between PGM and ceria. In the present paper, we describe the influence of newly developed washcoat components and PGM interaction with ceria on catalytic performance. First, to clear that the interaction between PGM and ceria contributes to catalytic performance, several kinds of catalysts which have the varied interactions between PGM and ceria were prepared using engineered washcoat techniques and evaluated in the model gas reactor. It was obvious that the difference in performance among them after aging derived from a diversity of interactions between Pt, Rh, and ceria. Second, for the purpose of determining the thermally durability of the developed Pt/Rh catalyst, the catalysts including the current catalyst were aged under three different temperatures and evaluated on engine dynamometer. Result of engine dynamometer evaluation revealed that significant improvement in the thermal durability can be achieved by optimizing the PGM-ceria interaction. In conclusion, we recognize that a thermal durability of a three-way catalyst can be improved by the stabilization of proper PGM-ceria interaction after aging as well as the utilization of thermally durable ceria material

  11. Synergistically Enhanced Electrochemical Performance of Ni3S4-PtX (X = Fe, Ni) Heteronanorods as Heterogeneous Catalysts in Dye-Sensitized Solar Cells.

    Science.gov (United States)

    Huang, Shoushuang; Ma, Dui; Hu, ZhangJun; He, Qingquan; Zai, Jiantao; Chen, Dayong; Sun, Huai; Chen, Zhiwen; Qiao, Qiquan; Wu, Minghong; Qian, Xuefeng

    2017-08-23

    Platinum (Pt)-based alloys are considerably promising electrocatalysts for the reduction of I - /I 3 - and Co 2+ /Co 3+ redox couples in dye-sensitized solar cells (DSSCs). However, it is still challenging to minimize the dosage of Pt to achieve comparable or even higher catalytic efficiency. Here, by taking full advantages of the Mott-Schottky (M-S) effect at the metal-semiconductor interface, we successfully strategize a low-Pt-based M-S catalyst with enhanced electrocatalytic performance and stability for the large-scale application of DSSCs. The optimized M-S electrocatalyst of Ni 3 S 4 -Pt 2 X 1 (X = Fe, Ni) heteronanorods is constructed by rationally controlling the ratio of Pt to transition metal in the hybrids. It was found that the electrons transferred from Ni 3 S 4 to Pt 2 X 1 at their interface under the Mott-Schottky effect result in the concentration of electrons onto Pt 2 X 1 domains, which subsequently accelerates the regeneration of both I - /I 3 - and Co 2+ /Co 3+ redox shuttles in DSSCs. As a result, the DSSC with Ni 3 S 4 -Pt 2 Fe 1 manifests an impressive power conversion efficiency (PCE) of 8.79% and 5.56% for iodine and cobalt-based electrolyte under AM1.5G illumination, respectively. These PCEs are obviously superior over those with Ni 3 S 4 -Pt, PtFe, Ni 3 S 4 , and pristine Pt electrodes. The strategy reported here is able to be further expanded to fabricate other low-Pt-alloyed M-S catalysts for wider applications in the fields of photocatalysis, water splitting, and heterojunction solar cells.

  12. 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.

  13. Enhancement of the electrooxidation of ethanol on Pt-Sn-P/C catalysts prepared by chemical deposition process

    Science.gov (United States)

    Xue, Xinzhong; Ge, Junjie; Tian, Tian; Liu, Changpeng; Xing, Wei; Lu, Tianhong

    In this paper, five Pt 3Sn 1/C catalysts have been prepared using three different methods. It was found that phosphorus deposited on the surface of carbon with Pt and Sn when sodium hypophosphite was used as reducing agent by optimization of synthetic conditions such as pH in the synthetic solution and temperature. The deposition of phosphorus should be effective on the size reduction and markedly reduces PtSn nanoparticle size, and raise electrochemical active surface (EAS) area of catalyst and improve the catalytic performance. TEM images show PtSnP nanoparticles are highly dispersed on the carbon surface with average diameters of 2 nm. The optimum composition is Pt 3Sn 1P 2/C (note PtSn/C-3) catalyst in my work. With this composition, it shows very high activity for the electrooxidation of ethanol and exhibit enhanced performance compared with other two Pt 3Sn 1/C catalysts that prepared using ethylene glycol reduction method (note PtSn/C-EG) and borohydride reduction method (note PtSn/-B). The maximum power densities of direct ethanol fuel cell (DEFC) were 61 mW cm -2 that is 150 and 170% higher than that of the PtSn/C-EG and PtSn/C-B catalyst.

  14. Enhancement of the electrooxidation of ethanol on Pt-Sn-P/C catalysts prepared by chemical deposition process

    Energy Technology Data Exchange (ETDEWEB)

    Xue, Xinzhong; Ge, Junjie; Tian, Tian [Changchun Institute of Applied Chemistry, Chinese Academy of Science, Changchun 130022 (China); Graduate University of the Chinese Academy of Sciences, Beijing 100049 (China); Liu, Changpeng; Xing, Wei; Lu, Tianhong [Changchun Institute of Applied Chemistry, Chinese Academy of Science, Changchun 130022 (China)

    2007-10-25

    In this paper, five Pt{sub 3}Sn{sub 1}/C catalysts have been prepared using three different methods. It was found that phosphorus deposited on the surface of carbon with Pt and Sn when sodium hypophosphite was used as reducing agent by optimization of synthetic conditions such as pH in the synthetic solution and temperature. The deposition of phosphorus should be effective on the size reduction and markedly reduces PtSn nanoparticle size, and raise electrochemical active surface (EAS) area of catalyst and improve the catalytic performance. TEM images show PtSnP nanoparticles are highly dispersed on the carbon surface with average diameters of 2 nm. The optimum composition is Pt{sub 3}Sn{sub 1}P{sub 2}/C (note PtSn/C-3) catalyst in my work. With this composition, it shows very high activity for the electrooxidation of ethanol and exhibit enhanced performance compared with other two Pt{sub 3}Sn{sub 1}/C catalysts that prepared using ethylene glycol reduction method (note PtSn/C-EG) and borohydride reduction method (note PtSn/-B). The maximum power densities of direct ethanol fuel cell (DEFC) were 61 mW cm{sup -2} that is 150 and 170% higher than that of the PtSn/C-EG and PtSn/C-B catalyst. (author)

  15. Facial synthesis of porous hematite supported Pt catalyst and its photo enhanced electrocatalytic ethanol oxidation performance

    International Nuclear Information System (INIS)

    Kang, Shuai; Shen, Pei Kang

    2015-01-01

    Graphical Abstract: A porous α-Fe 2 O 3 supported Pt catalyst has been synthesized by a facial thermal treatment assisted precipitation method and the materials show a illumination enhanced performance for ethanol oxidation. Display Omitted -- Highlights: •A porous α-Fe 2 O 3 supported Pt catalyst has been synthesized for the first time. •With the addition of α-Fe 2 O 3 , the current density of Pt/C grows about 51% under illumination and 32% in the dark compared with unsupported catalyst. •The current increases under illuminationin chronoamperometric experiments at a given potential of 0.7 V due to the photons from light provide energy for CO stripping. •This work demostrates an optical strategy to accelerate electrode reactions towards ethanol oxidation reaction. -- Abstract: The porous α-Fe 2 O 3 supported Pt catalyst is synthesized by a facial thermal treatment assisted precipitation method. The particle size of Pt is less than 3 nm. The pore diameters of α-Fe 2 O 3 particles are concentrated to 2.46 nm in a mesooporous scale. Its electrochemical performance is tested. The ethanol oxidation current of the Pt/Fe 2 O 3 catalsyt obviously improves under illumination, compared with that in the dark, during the optical switching operation. Moreover, with the addition of α-Fe 2 O 3 , the ethanol oxidation current of Pt/C grows about 51% under illumination and 32% in the dark; the onset potential shifts negtively for about 20 mV. This work demostrates an optical strategy which can be a potential alternative to accelerate electrode reactions towards ethanol oxidation reaction

  16. Reaction mechanism of ethylene glycol decomposition on Pt model catalysts: A density functional theory study

    International Nuclear Information System (INIS)

    Lv, Cun-Qin; Yang, Bo; Pang, Xian-Yong; Wang, Gui-Chang

    2016-01-01

    Highlights: • DFT calculations were performed to study the ethylene glycol decomposition on Pt. • The final products are CO and H_2 on Pt(111), (100) and (211). • Ethylene glycol decomposition on Pt(111) undergoes via initial O−H bond scission and followed by C−H bond cleavage. • Ethylene glycol decomposition proceeds via initial O−H bond scission and followed by O−H bond cleavage on Pt(100)/(211). - Abstract: Understanding and controlling bond beak sequence is important in catalytic processes. The DFT-GGA method combined with slab model was performed to study the ethylene glycol decomposition on various Pt model catalysts such as close-packed Pt(111), stepped Pt(211) and a more open one, Pt(100). Calculation results show that the adsorption energies of ethylene glycol and other decomposition species depend on the coordination number of surface atom, that is, low coordination number correspond to high adsorption energy. Moreover, it was found that final products of ethylene glycol decomposition are CO and H_2 on all model catalysts, but the reaction mechanism varies: On Pt(111), the first step is O−H bond scission, followed by C−H bond cleavage, namely C_2H_6O_2 → HOCH_2CH_2O + H → HOCH_2CHO + 2H→ HOCH_2CO +3H → OCH_2CO + 4H → OCHCO + 5H → CO + HCO + 5H → 2CO + 6H→ 2CO + 3H_2; On Pt(211) and Pt(100), however, it is a second O−H bond cleavage that follows the initial O−H bond scission, that is, C_2H_6O_2 → HOCH_2CH_2O + H → OCH_2CH_2O + 2H → OCHCH_2O + 3H → OCHCHO + 4H → 2HCO + 4H → 2CO + 6H → 2CO + 3H_2  on Pt(211), and C_2H_6O_2 →HOCH_2CH_2O+ H → OCH_2CH_2O + 2H→OCHCH_2O+3H→OCCH_2O+4H→CO+H_2CO+4H→CO+HCO+5H→2CO+6H→2CO+3H_2 on Pt(100) For the catalytic order of ethylene glycol to form H_2, it may be determined based on the rate-controlling step, and it is Pt(111) > Pt(211) > Pt(100).

  17. 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)

  18. An Analysis of Logistics Efficiency in PT. XYZ Surabaya Branch

    OpenAIRE

    Leevana, Elyn

    2015-01-01

    Logistic efficiency is an important element in enhancement of company's competitiveness. Therefore, this research is conducted to investigate factors that influence logistics efficiency using the study case from PT. XYZ. PT. XYZ is a company in distribution industry that distributes palm oil products and other food products from the manufacturer to retail businesses. The researcher will analyze factors that influence logistics efficiency, measured by transportation costs in this research.Rese...

  19. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2007-12-01

    Novel carbon supported Pt/SnO{sub x}/C catalysts with Pt:Sn atomic ratios of 5:5, 6:4, 7:3 and 8:2 were prepared by a modified polyol method and characterized with respect to their structural properties (X-ray diffraction (XRD) and transmission electron microscopy (TEM)), chemical composition (XPS), their electrochemical properties (base voltammetry, CO{sub ad} stripping) and their electrocatalytic activity and selectivity for ethanol oxidation (ethanol oxidation reaction (EOR)). The data show that the Pt/SnO{sub x}/C catalysts are composed of Pt and tin oxide nanoparticles with an average Pt particle diameter of about 2 nm. The steady-state activity of the Pt/SnO{sub x}/C catalysts towards the EOR decreases with tin content at room temperature, but increases at 80 deg. C. On all Pt/SnO{sub x}/C catalysts, acetic acid and acetaldehyde represent dominant products, CO{sub 2} formation contributes 1-3% for both potentiostatic and potentiodynamic reaction conditions. With increasing potential, the acetaldehyde yield decreases and the acetic acid yield increases. The apparent activation energies of the EOR increase with tin content (19-29 kJ mol{sup -1}), but are lower than on Pt/C (32 kJ mol{sup -1}). The somewhat better performance of the Pt/SnO{sub x}/C catalysts compared to alloyed PtSn{sub x}/C catalysts is attributed to the presence of both sufficiently large Pt ensembles for ethanol dehydrogenation and C-C bond splitting and of tin oxide for OH generation. Fuel cell measurements performed for comparison largely confirm the results obtained in model studies.

  1. Hydrogenation of fructose to 2,5-dimethyltetrahydrofuran using a sulfur poisoned Pt/C catalyst

    Science.gov (United States)

    In order to expand the number of biobased chemicals available, fructose has been hydrogenated to 2,5-dimethyltetrahydrofuran using a sulfided Pt/C catalyst. The reaction was carried out in a stirred reactor at 10.3 MPa H2 and 175°C which allowed a 10% fructose solution to be converted in about 2 h. ...

  2. Hydrodeoxygenation of waste fat for diesel production: Study on model feed with Pt/alumina catalyst

    DEFF Research Database (Denmark)

    Madsen, Anders Theilgaard; Ahmed, El Hadi; Christensen, Claus H.

    2011-01-01

    Hydrodeoxygenation of waste fats and oils is a viable method for producing renewable diesel oil. In this study a model feed consisting of oleic acid and tripalmitin in molar ratio 1:3 was hydrotreated at 325°C with 20bars H2 in a stirred batch autoclave with a 5wt% Pt/γ-Al2O3 catalyst, and samples...

  3. Preparation of Pt-SDB hydrophobic catalyst used in H2-H2O isotope exchange reaction

    International Nuclear Information System (INIS)

    Li Junhua; Kang Yi; Ruan Hao; Dou Qincheng; Han Yande; Hu Shilin

    2001-01-01

    The preparation of Pt-SDB hydrophobic catalyst is studied, in which platinum as active metal and polystyrene divinylbenzene (SDB) as the carrier. Hydrogen isotope exchange reaction is carried out with Pt-SDB catalyst in counter-current in the trickle bed. The effect of preparing condition on the activity of catalyst is discussed. The results show that the excellent catalyst is obtained by reduced at the temperature of 200 degree C over 8 hours. Hydrophobic catalyst is high activity and stability as the amount of platinum content is 3%, the platinum can reach the economic use with the content of (1-2)%

  4. Highly Selective TiN-Supported Highly Dispersed Pt Catalyst: Ultra Active toward Hydrogen Oxidation and Inactive toward Oxygen Reduction.

    Science.gov (United States)

    Luo, Junming; Tang, Haibo; Tian, Xinlong; Hou, Sanying; Li, Xiuhua; Du, Li; Liao, Shijun

    2018-01-31

    The severe dissolution of the cathode catalyst, caused by an undesired oxygen reduction reaction at the anode during startup and shutdown, is a fatal challenge to practical applications of polymer electrolyte membrane fuel cells. To address this important issue, according to the distinct structure-sensitivity between the σ-type bond in H 2 and the π-type bond in O 2 , we design a HD-Pt/TiN material by highly dispersing Pt on the TiN surface to inhibit the unwanted oxygen reduction reaction. The highly dispersed Pt/TiN catalyst exhibits excellent selectivity toward hydrogen oxidation and oxygen reduction reactions. With a Pt loading of 0.88 wt %, our catalyst shows excellent hydrogen oxidation reaction activity, close to that of commercial 20 wt % Pt/C catalyst, and much lower oxygen reduction reaction activity than the commercial 20 wt % Pt/C catalyst. The lack of well-ordered Pt facets is responsible for the excellent selectivity of the HD-Pt/TiN materials toward hydrogen oxidation and oxygen reduction reactions. Our work provides a new and cost-effective solution to design selective catalysts toward hydrogen oxidation and oxygen reduction reactions, making the strategy of using oxygen-tolerant anode catalyst to improve the stability of polymer electrolyte membrane fuel cells during startup and shutdown more affordable and practical.

  5. High Coke-Resistance Pt/Mg1-xNixO Catalyst for Dry Reforming of Methane.

    Directory of Open Access Journals (Sweden)

    Faris A J Al-Doghachi

    Full Text Available A highly active and stable nano structured Pt/Mg1-xNixO catalysts was developed by a simple co-precipitation method. The obtained Pt/Mg1-xNixO catalyst exhibited cubic structure nanocatalyst with a size of 50-80 nm and realized CH4 and CO2 conversions as high as 98% at 900°C with excellent stability in the dry reforming of methane. The characterization of catalyst was performed using various kinds of analytical techniques including XRD, BET, XRF, TPR-H2, TGA, TEM, FESEM, FT-IR, and XPS analyses. Characterization of spent catalyst further confirms that Pt/Mg1-xNixO catalyst has high coke-resistance for dry reforming. Thus, the catalyst demonstrated in this study, offers a promising catalyst for resolving the dilemma between dispersion and reducibility of supported metal, as well as activity and stability during high temperature reactions.

  6. Cobalt hydroxide film on Pt as co-catalyst for oxidation of polyhydric alcohols in alkaline medium

    International Nuclear Information System (INIS)

    Das, Debasmita; Das, Kaushik

    2010-01-01

    Electrochemical behavior of chemically prepared Co(OH) 2 film on Pt has been studied in alkaline medium using cyclic voltammetry and chronoamperometry. Amount of Co(OH) 2 deposited increases linearly with the number of times of deposition. The deposit is of fibrous structure, as shown by scanning electron microphotograph. There is evidence of Co II /Co III and Co III /Co IV redox transitions during the cyclic potential scan. The former oxidation proceeds under diffusion control. The Co(OH) 2 deposit acts as an efficient co-catalyst for anodic oxidation of ethanediol, propanediol and glycerol on Pt in alkaline medium. This is demonstrated by appreciable enhancement of the alcohol oxidation currents upon deposition of Co(OH) 2 on Pt. Among the alcohols studied, the highest oxidation currents are obtained for ethanediol, both on Co(OH) 2 /Pt and bare Pt. Co(OH) 2 alone also acts as a redox mediator for alcohol oxidation at more positive potentials.

  7. Titania Supported Pt and Pt/Pd Nano-particle Catalysts for the Oxidation of Sulfur Dioxide

    DEFF Research Database (Denmark)

    Koutsopoulos, Sotiris; Johannessen, Tue; Eriksen, Kim Michael

    2006-01-01

    Several types of titania (anatase) were used as supports for pure platinum and Pt–Pd bimetallic alloy catalysts. The preparation methods, normal wet impregnation technique and flame aerosol synthesis, obtained metal loadings of 2% by weight. The prepared catalysts were tested for SO2 oxidation...... activity at atmospheric pressure in the temperature range 250–600 °C. The SO2 to SO3 conversion efficiency of the Pt–Pd alloy was significantly higher than that of the individual metals. The effects of the preparation method and the titania type used on the properties and activity of the resulting catalyst...

  8. New proposition on performance evaluation of hydrophobic Pt catalyst packed in trickle bed

    International Nuclear Information System (INIS)

    Shimizu, Masami; Kitamoto, Asashi; Takashima, Yoichi.

    1983-01-01

    On the evaluation of the performance of the hydrophobic Pt catalyst packed in the trickle-bed test column, the conventionally defined (Ksub(y)a) and the newly defined (Ksub(f))sub (G) are compared with each other as a measure of the overall D-transfer coefficient. The value of (Ksub(y)a) varies in a wide range in accordance with the length of the test column. On the other hand (Ksub(f))sub (G sub (l = L)) has a finite value in the test column longer than about 0.5 m. By considering the values of ksub(g) and ksub(l) which are the constituents of (Ksub(f))sub (G), it is possible to improve the hydrophobic Pt catalyst trickle bed and to design the H 2 /H 2 O-isotopic exchange trickle-bed column packed with this catalyst. (author)

  9. Activity of bimetallic catalysts (Pt + Me)/A12030 in butane hydrogenolysis and benzene hydrogenation

    International Nuclear Information System (INIS)

    Zharkov, B.B.; Rubinov, A.Z.

    1986-01-01

    The authors evaluate the decomposing and hydrogenating activity of some Me/Al 2 0 3 0 and (Pt + Me)/Al 203 catalysis for the reactions of butane hydrogenolysis and conversion of benzene to cyclohexane. The temperature was 180-300 C for butane transformation and 150 C for benzene hydrogenation. During both reactions some initial decrease of catalytic activity which stabilized over 2-3 h was observed. The results show that roasting Re-containing reforming catalysts at fairly high temperatures (500-550 C) balances maximum hydrogenating and average splitting activities, thus guaranteeing high resistance to coke deposition while preserving the necessary selectivity. The decreased hydrogenating capacity of Ir/A1 2 0 3 0 and (Pt + Ir)/A1 23 0 catalysts after roasting at 500 C indicates insufficient thermal stability, which can be why renewing the initial activity of iridium containing forming catalysts by oxidating regeneration is difficult

  10. Synthesis of Pt@TiO2@CNTs Hierarchical Structure Catalyst by Atomic Layer Deposition and Their Photocatalytic and Photoelectrochemical Activity.

    Science.gov (United States)

    Liao, Shih-Yun; Yang, Ya-Chu; Huang, Sheng-Hsin; Gan, Jon-Yiew

    2017-04-29

    Pt@TiO2@CNTs hierarchical structures were prepared by first functionalizing carbon nanotubes (CNTs) with nitric acid at 140 °C. Coating of TiO2 particles on the CNTs at 300 °C was then conducted by atomic layer deposition (ALD). After the TiO2@CNTs structure was fabricated, Pt particles were deposited on the TiO2 surface as co-catalyst by plasma-enhanced ALD. The saturated deposition rates of TiO2 on a-CNTs were 1.5 Å/cycle and 0.4 Å/cycle for substrate-enhanced process and linear process, respectively. The saturated deposition rate of Pt on TiO2 was 0.39 Å/cycle. The photocatalytic activities of Pt@TiO2@CNTs hierarchical structures were higher than those without Pt co-catalyst. The particle size of Pt on TiO2@CNTs was a key factor to determine the efficiency of methylene blue (MB) degradation. The Pt@TiO2@CNTs of 2.41 ± 0.27 nm exhibited the best efficiency of MB degradation.

  11. Regeneration of Pt-catalysts deactivated in municipal waste flue gas with H2/N2 and the effect of regeneration step on the SCR catalyst

    DEFF Research Database (Denmark)

    Due-Hansen, Johannes; Rasmussen, Søren Brik; Kustov, Arkady

    The deactivation performance of Pt-catalysts for CO oxidation has been studied in relation to use in sewage sludge municipal waste burners, where HMDS was found to poison the industrial catalyst in a similar way to the model Pt/TiO2 catalyst. A promising regeneration procedure was developed based...... on reduction with hydrogen. This procedure had negligible effect on the performance of the SCR catalyst. After treatment with 2% H2, 8% O2 in N2 for one hour, a slight better NO SCR activity was observed due to increase in the concentration V4+ sites. However, after exposure in normal NO SCR gases the activity...

  12. Enhanced methanol electro-oxidation reaction on Pt-CoOx/MWCNTs hybrid electro-catalyst

    International Nuclear Information System (INIS)

    Nouralishahi, Amideddin; Rashidi, Ali Morad; Mortazavi, Yadollah; Khodadadi, Abbas Ali; Choolaei, Mohammadmehdi

    2015-01-01

    Highlights: • Promoting effects of Cobalt oxide on methanol electro-oxidation over Pt/MWCNTs are investigated. • Higher activity, about 2.9 times, and enhanced stability are observed on Pt-CoO x /MWCNTs. • Electrochemical active surface area of Pt nanoparticles is significantly improved upon CoO x addition. • Bi-functional mechanism is facilitated in presence of CoO x . - Abstract: The electro-catalytic behavior of Pt-CoO x /MWCNTs in methanol electro-oxidation reaction (MOR) is investigated and compared to that of Pt/MWCNTs. The electro-catalysts were synthesized by an impregnation method using NaBH 4  as the reducing agent. The morphological and physical characteristics of samples are examined by XRD, TEM, ICP and EDS techniques. In the presence of CoO x , Pt nanoparticles were highly distributed on the support with an average particle size of 2 nm, an obvious decrease from 5.1 nm for Pt/MWCNTs. Cyclic voltammetry, CO-stripping, Chronoamperometry, and electrochemical impedance spectroscopy (EIS) measurements are used to study the electrochemical behavior of the electro-catalysts. The results revealed a considerable enhancement in the oxidation kinetics of CO ads on Pt active sites by the participation of CoO x . Compared to Pt/MWCNTs, Pt-CoO x /MWCNTs sample has a larger electrochemical active surface area (ECSA) and higher electro-catalytic activity and stability toward methanol electro-oxidation. According to the results of cyclic voltammetry, the forward anodic peak current density enhances more than 89% at the optimum atomic ratio of Pt:Co = 2:1. Furthermore, inclusion of cobalt oxide species causes the onset potential of methanol electro-oxidation reaction to shift 84 mV to negative values compared to that on Pt/MWCNTs. Based on EIS data, dehydrogenation of methanol is the rate-determining step of MOR on both Pt/MWCNTs and Pt-CoO x /MWCNTs, at small overpotentials. However, at higher overpotentials, the oxidation of adsorbed oxygen-containing groups

  13. Pt based PEMFC catalysts prepared from colloidal particle suspensions--a toolbox for model studies.

    Science.gov (United States)

    Speder, Jozsef; Altmann, Lena; Roefzaad, Melanie; Bäumer, Marcus; Kirkensgaard, Jacob J K; Mortensen, Kell; Arenz, Matthias

    2013-03-14

    A colloidal synthesis approach is presented that allows systematic studies of the properties of supported proton exchange membrane fuel cell (PEMFC) catalysts. The applied synthesis route is based on the preparation of monodisperse nanoparticles in the absence of strong binding organic stabilizing agents. No temperature post-treatment of the catalyst is required rendering the synthesis route ideally suitable for comparative studies. We report work concerning a series of catalysts based on the same colloidal Pt nanoparticle (NP) suspension, but with different high surface area (HSA) carbon supports. It is shown that for the prepared catalysts the carbon support has no catalytic co-function, but carbon pre-treatment leads to enhanced sticking of the Pt NPs on the support. An unwanted side effect, however, is NP agglomeration during synthesis. By contrast, enhanced NP sticking without agglomeration can be accomplished by the addition of an ionomer to the NP suspension. The catalytic activity of the prepared catalysts for the oxygen reduction reaction is comparable to industrial catalysts and no influence of the particle size is found in the range of 2-5 nm.

  14. CO Sensing Performance of a Micro Thermoelectric Gas Sensor with AuPtPd/SnO2 Catalyst and Effects of a Double Catalyst Structure with Pt/α-Al2O3

    Science.gov (United States)

    Goto, Tomoyo; Itoh, Toshio; Akamatsu, Takafumi; Shin, Woosuck

    2015-01-01

    The CO sensing properties of a micro thermoelectric gas sensor (micro-TGS) with a double AuPtPd/SnO2 and Pt/α-Al2O3 catalyst were investigated. While several nanometer sized Pt and Pd particles were uniformly dispersed on SnO2, the Au particles were aggregated as particles measuring >10 nm in diameter. In situ diffuse reflectance Fourier transform Infrared spectroscopy (DRIFT) analysis of the catalyst showed a CO adsorption peak on Pt and Pd, but no clear peak corresponding to the interaction between CO and Au was detected. Up to 200 °C, CO combustion was more temperature dependent than that of H2, while H2 combustion was activated by repeated exposure to H2 gas during the periodic gas test. Selective CO sensing of the micro-TGS against H2 was attempted using a double catalyst structure with 0.3–30 wt% Pt/α-Al2O3 as a counterpart combustion catalyst. The sensor output of the micro-TGS decreased with increasing Pt content in the Pt/α-Al2O3 catalyst, by cancelling out the combustion heat from the AuPtPd/SnO2 catalyst. In addition, the AuPtPd/SnO2 and 0.3 wt% Pt/α-Al2O3 double catalyst sensor showed good and selective CO detection. We therefore demonstrated that our micro-TGS with double catalyst structure is useful for controlling the gas selectivity of CO against H2. PMID:26694397

  15. Pt -based anode catalysts for direct ethanol fuel cells

    International Nuclear Information System (INIS)

    Hoyos, Bibian; Sanchez, Carlos; Gonzalez, Javier

    2007-01-01

    In this work it is studied the electro-catalytic behavior of pure platinum and platinum-based alloys with Ru, Sn, Ir, and Os supported on carbon to the ethanol electro-oxidation in aims to develop anodic catalysts for direct ethanol fuel cells, additionally, porous electrodes and membrane electrode assemblies were built for proton exchange membrane fuel cells in which the electrodes were tested. Catalysts characterization was made by cyclic voltammetry whereas the fuel cells behavior tests were made by current-potential polarization curves. in general, all alloys show a lower on-set reaction potential and a higher catalytic activity than pure platinum. However, in the high over potential zone, pure platinum has higher catalytic activity than the alloys. In agreement with these results, the alloys studied here could be useful in fuel cells operating on moderated and low current

  16. A general protocol for the synthesis of Pt-Sn/C catalysts for the ethanol electrooxidation reaction

    Energy Technology Data Exchange (ETDEWEB)

    Liu, B.; Lee, Z.Y.; Cheng, C.H.; Lee, J.Y. [Chemical and Biomolecular Engineering, National University of Singapore (Singapore); Chia, Z.W. [NUS Graduate School for Integrative Sciences and Engineering (NGS), Centre for Life Sciences (CeLS), Singapore (Singapore); Liu, Z.L. [Institute of Materials Research and Engineering, 3 Research Link, Singapore 117602 (Singapore)

    2012-08-15

    A general protocol for the synthesis of Pt-Sn/C catalysts for ethanol electrooxidation by the polyol method is developed after a systematic variation of the preparation variables. This protocol enables the complete transfer of all catalytic elements in the preparation solution to the catalyst support; thereby providing a convenient means of catalyst composition control. Water is a necessary co-solvent for ethylene glycol in the polyol synthesis of Pt-Sn/C catalysts. The best preparation medium for controlling the particle size to small sizes is 0.1 M NaOH solution in a mixture of equal volumes of water and ethylene glycol. With this medium composition Pt-Sn/C catalysts with the optimized target Pt:Sn atomic ratio of 3:1 could be expeditiously prepared for ethanol electrooxidation. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

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

    Directory of Open Access Journals (Sweden)

    Feng Li

    2018-02-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-10-06

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

  19. 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.

  20. Preparation and characterization of Pt-Sn/C and Pt-Ir/C catalysts for the electrochemical oxidation of ethanol in polymer electrolyte membrane fuel cell

    CSIR Research Space (South Africa)

    Masombuka, T

    2007-11-01

    Full Text Available oxidation is still low. Development of new active catalysts able to break C-C bond and complete oxidation of ethanol into CO 2 is of fundamental importance. Generally, a third metal is added to the best binary Pt-Sn catalyst to improve CO tolerance...

  1. Efficient epoxidation of propene using molecular catalysts

    DEFF Research Database (Denmark)

    Markovits, Iulius I. E.; Anthofer, Michael H.; Kolding, Helene

    2014-01-01

    The epoxidation of propene is performed in homogeneous phase using various molecular catalysts and H2O2 or tert-butyl hydroperoxide as oxidants. A comparison between some molybdenum catalysts and methyltrioxorhenium (MTO) shows that the well known Re catalyst is the best among the examined...

  2. Synthesis and characterization of Pt-Sn-Ni alloys to application as catalysts for direct ethanol fuel cells; Sintese e caracterizacao de ligas de Pt-Sn-Ni para aplicacao como caztalisadores em celulas a combustivel do tipo DEFC

    Energy Technology Data Exchange (ETDEWEB)

    Silva, E.L. da; Correa, P.S.; Oliveira, E.L. de; Takimi, A.S.; Malfatti, C.F., E-mail: celia.malfatti@ufrgs.b [Universidade Federal do Rio Grande do Sul (LAPEC/UFRGS), Porto Alegre, RS (Brazil). Programa de Pos-Graduacao em Engenharia Mecanica. Lab. de Pesquisa em Corrosao; Radtke, C. [Universidade Federal do Rio Grande do Sul (IQ/UFRGS), Porto Alegre, RS (Brazil). Inst. de Quimica

    2010-07-01

    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)

  3. Crumpled rGO-supported Pt-Ir bifunctional catalyst prepared by spray pyrolysis for unitized regenerative fuel cells

    Science.gov (United States)

    Kim, In Gyeom; Nah, In Wook; Oh, In-Hwan; Park, Sehkyu

    2017-10-01

    Three-dimensional (3D) crumpled reduced graphene oxide supported Pt-Ir alloys that served as bifunctional oxygen catalysts for use in untized regenerative fuel cells were synthesized by a facile spray pyrolysis method. Pt-Ir catalysts supported on rGO (Pt-Ir/rGOs) were physically characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and thermogravimetric analysis (TGA) to observe change in composition by heat treatment, alloying, and morphological transition of the catalysts. Their catalytic activities and stabilities for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) conditions were electrochemically investigated using cyclic voltammetry (CV), linear sweep voltammetry (LSV), potential cycling and hold tests on the rotating disk electrode (RDE). Pt-Ir/rGO with no post heat-treatment (Pt-Ir/rGO_NP) showed a lower activity for ORR and OER although metal nanoparticles decorated on the support are relatively small. However, Pt-Ir/rGO showed remarkably enhanced activity following heat treatment, depending on temperature. Pt-Ir/rGO heat-treated at 600 °C after spray pyrolysis (Pt-Ir/rGO_P600) exhibited a higher activity and stability than a commercially available Pt/C catalyst kept under the ORR condition, and it also revealed a comparable OER activity and durability versus the commercial unsupported Ir catalyst.

  4. 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.

  5. Effect of the structural characteristics of binary Pt-Ru and ternary Pt-Ru-M fuel cell catalysts on the activity of ethanol electrooxidation in acid medium.

    Science.gov (United States)

    Antolini, Ermete

    2013-06-01

    In view of their possible use as anode materials in acid direct ethanol fuel cells, the electrocatalytic activity of Pt-Ru and Pt-Ru-M catalysts for ethanol oxidation has been investigated. This minireview examines the effects of the structural characteristics of Pt-Ru, such as the degree of alloying and Ru oxidation state, on the electrocatalytic activity for ethanol oxidation. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  6. Pt-Ni/WC Alloy Nanorods Arrays as ORR Catalyst for PEM Fuel Cells

    Energy Technology Data Exchange (ETDEWEB)

    Begum, Mahbuba; Yurukcu, Mesut; Yurtsever, Fatma; Ergul, Busra; Kariuki, Nancy; Myers, Deborah J.; Karabacak, Tansel

    2017-08-24

    Polymer electrolyte membrane fuel cells (PEMFCs) among the other types of fuel cell technology are attractive power sources, especially for electric vehicle applications. While significant progress and plausible prospects of PEMFCs have been achieved, there are still some challenges related to the performance, durability, and cost that need to be overcome to make them economically viable for widespread commercialization. Our strategy is to develop thin films of high-active and stable catalyst coated on vertically aligned nanorod arrays of conductive and stable support. In this work, we fabricated tungsten carbide (WC) nanorods as support and coated them with a platinum-nickel (Pt-Ni) alloy shell denoted as Pt-Ni/WC catalysts. The Pt- Ni/WC nanorods were deposited on glassy carbon disks as well as on silicon substrates for evaluation of their electrocatalytic oxygen reduction reaction (ORR) activity and physical properties. Cyclic voltammetry experiments using rotating disk electrode were performed in perchloric acid (0.1 M HClO4) electrolyte at room temperature to characterize the ORR activity and stability of Pt-Ni/WC nanorods catalysts. Scanning electron microscopy and X-ray diffraction techniques were utilized to study the morphology and crystallographic properties, respectively.

  7. Mesoporous PtSnO2/C Catalyst with Enhanced Catalytic Activity for Ethanol Electro-oxidation

    Directory of Open Access Journals (Sweden)

    Siyu Chen

    2018-01-01

    Full Text Available In this paper, we report the synthesis, characterization, and electrochemical evaluation of a mesoporous PtSnO2/C catalyst, called PtSnO2(M/C, with a nominal Pt : Sn ratio of 3 : 1. Brunauer–Emmett–Teller and transmission electron microscopy characterizations showed the obvious mesoporous structure of SnO2 in PtSnO2(M/C catalyst. X-ray photoelectron spectroscopy analysis exhibited the interaction between Pt and mesoporous SnO2. Compared with Pt/C and commercial PtSnO2/C catalysts, PtSnO2(M/C catalyst has a lower active site, but higher catalytic activity for ethanol electro-oxidation reaction (EOR. The enhanced activity could be attributed to Pt nanoparticles deposited on mesoporous SnO2 that could decrease the amount of poisonous intermediates produced during EOR by the interaction between Pt and mesoporous SnO2.

  8. 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.

  9. Oxidation of Propylene on catalytic Pt-Cu/y alumina. (Part I) Characterization of catalysts of Pt-Cu/y alumina for chemisorption of H2

    International Nuclear Information System (INIS)

    Carballo, Luis M; Zea, Hugo R

    1999-01-01

    In this work the effect of the composition of catalysts of Pt-Cu/y-alumina is analyzed on the superficial area it reactivates corresponding to the total oxidation of propylene. The experimental essays were also made in a differential reactor that was used so much for the characterization of the catalyst in situ by means of the measurement of the selective chemisorption of H 2 , the effects and the bimetallic interactions are discussed that frequently happen in the supported catalysts. Starting from the studies of chemical adsorption of H 2 on the supported catalysts of Pt-Cu was, by means of the application of the theory of the regular solution to the surface of the glasses and keeping in mind that the H 2 it adsorbs chemically only on the superficial atoms of Pt (it was observed that the hydrogen not it chemi-absorb on the Cu) that the Cu atoms are segregated to the surface of the bimetallic crystals

  10. Engineering Ru@Pt Core-Shell Catalysts for Enhanced Electrochemical Oxygen Reduction Mass Activity and Stability.

    Science.gov (United States)

    Jackson, Ariel; Strickler, Alaina; Higgins, Drew; Jaramillo, Thomas Francisco

    2018-01-12

    Improving the performance of oxygen reduction reaction (ORR) electrocatalysts is essential for the commercial efficacy of many renewable energy technologies, including low temperature polymer electrolyte fuel cells (PEFCs). Herein, we report highly active and stable carbon-supported Ru@Pt core-shell nanoparticles (Ru@Pt/C) prepared by a wet chemical synthesis technique. Through rotating disc electrode testing, the Ru@Pt/C achieves an ORR Pt mass-based activity of 0.50 A mg Pt -1 at 0.9 V versus the reversible hydrogen electrode (RHE), which exceeds the activity of the state-of-the-art commercial Pt/C catalyst as well as the Department of Energy 2020 PEFC electrocatalyst activity targets for transportation applications. The impact of various synthetic parameters, including Pt to Ru ratios and catalyst pretreatments (i.e., annealing) are thoroughly explored. Pt-based mass activity of all prepared Ru@Pt/C catalysts was found to exceed 0.4 mg Pt -1 across the range of compositions investigated, with the maximum activity catalyst having a Ru:Pt ratio of 1:1. This optimized composition of Ru@Pt/C catalyst demonstrated remarkable stability after 30,000 accelerated durability cycles (0.6 to 1.0 V vs. RHE at 125 mV s -1 ), maintaining 85% of its initial mass activity. Scanning transmission electron microscopy energy dispersive spectroscopy (STEM-EDS) analysis at various stages of electrochemical testing demonstrated that the Pt shell can provide sufficient protection against the dissolution of the otherwise unstable Ru core.

  11. Diethyl Ether Production during Catalytic Dehydration of Ethanol over Ru- and Pt- modified H-beta Zeolite Catalysts.

    Science.gov (United States)

    Kamsuwan, Tanutporn; Praserthdam, Piyasan; Jongsomjit, Bunjerd

    2017-01-01

    In the present study, the catalytic dehydration of ethanol over H-beta zeolite (HBZ) catalyst with ruthenium (Ru-HBZ) and platinum (Pt-HBZ) modification was investigated. Upon the reaction temperature between 200 and 400°C, it revealed that ethanol conversion and ethylene selectivity increased with increasing temperature for both Ru and Pt modification. At lower temperature (200 to 250°C), diethyl ether (DEE) was the major product. It was found that Ru and Pt modification on HBZ catalyst can result in increased DEE yield at low reaction temperature due to increased ethanol conversion without a significant change in DEE selectivity. By comparing the DEE yield of all catalysts in this study, the Ru-HBZ catalyst apparently exhibited the highest DEE yield (ca. 47%) at 250°C. However, at temperature from 350 to 400°C, the effect of Ru and Pt was less pronounced on ethylene yield. With various characterization techniques, the effects of Ru and Pt modification on HBZ catalyst were elucidated. It revealed that Ru and Pt were present in the highly dispersed forms and well distributed in the catalyst granules. It appeared that the weak acid sites measured by NH 3 temperature-programmed desorption technique also decreased with Ru and Pt promotion. Thus, the increased DEE yields with the Ru and Pt modification can be attributed to the presence of optimal weak acid sites leading to increased intrinsic activity of the catalysts. It can be concluded that the modification of Ru and Pt on HBZ catalyst can improve the DEE yields by ca. 10%.

  12. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-07-01

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

  14. Practical chemical analysis of Pt and Pd based heterogeneous catalysts with hard X-ray photoelectron spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Yoshikawa, H., E-mail: YOSHIKAWA.Hideki@nims.go.jp [National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047 (Japan); Matolínová, I.; Matolín, V. [Charles University in Prague, Faculty of Mathematics and Physics, V Holešovičkách 2, 18000 Prague 8 (Czech Republic)

    2013-10-15

    Highlights: •Hard X-ray photoelectron spectroscopy (HAXPES) enables interface analysis of catalyst. •HAXPES enables overall analysis of porous film of Pt-doped CeO{sub 2} and related catalyst. •HAXPES enables analysis of trace elements for Pd and Pt{sub 3}Ni nanoparticle catalysts. -- Abstract: Interfacial properties including configuration, porosity, chemical states, and atomic diffusion greatly affect the performance of supported heterogeneous catalysts. Hard X-ray photoelectron spectroscopy (HAXPES) can be used to analyze the interfaces of heterogeneous catalysts because of its large information depth of more than 20 nm. We use HAXPES to examine Pt-doped CeO{sub 2} and related thin film catalysts evaporated on Si, carbon, and carbon nanotube substrates, because Pt-doped CeO{sub 2} has great potential as a noble metal-based heterogeneous catalyst for fuel cells. The HAXPES measurements clarify that the dopant material, substrate material, and surface pretreatment of substrate are important parameters that affect the interfacial properties of Pt-doped CeO{sub 2} and related thin film catalysts. Another advantage of HAXPES measurement of heterogeneous catalysts is that it can be used for chemical analysis of trace elements by detecting photoelectrons from deep core levels, which have large photoionization cross-sections in the hard X-ray region. We use HAXPES for chemical analysis of trace elements in Pd nanoparticle catalysts immobilized on sulfur-terminated substrates and Pt{sub 3}Ni nanoparticle catalysts enveloped by dendrimer molecules.

  15. Low temperature catalytic combustion of propane over Pt-based catalyst with inverse opal microstructure in microchannel reactor

    NARCIS (Netherlands)

    Guan, G.; Zapf, R.; Kolb, G.A.; Men, Y.; Hessel, V.; Löwe, H.; Ye, J.; Zentel, R.

    2007-01-01

    novel Pt-based catalyst with highly regular, periodic inverse opal microstructure was fabricated in a microchannel reactor, and catalytic testing revealed excellent conversion and stable activity for propane combustion at low temperatures

  16. Enhanced Activity and Durability of Nanosized Pt-SnO2/IrO2/CNTs Catalyst for Methanol Electrooxidation.

    Science.gov (United States)

    Wang, Hongjuan; Wang, Xiaohui; Zheng, Jiadao; Peng, Feng; Yu, Hao

    2015-05-01

    Pt-SnO2/IrO2/CNTs anode catalyst for direct methanol fuel cell was designed and prepared with IrO2/CNTs as support for the subsequent immobilization of Pt and SnO2 at the same time. The structure of the catalysts and their catalytic performance in methanol electrooxidation were investigated and the roles of IrO2 and SnO2 in methanol electrooxidation were discussed as well. Results show that Pt-SnO2/IrO2/CNTs catalyst exhibits the best activity and durability for methanol electrooxidation when compared with Pt/CNTs, Pt/IrO2/CNTs and Pt-SnO2/CNTs. According to the results of electrochemical tests and physicochemical characterizations, the enhancements of Pt-SnO2/IrO2/CNTs were attributed to the special properties of IrO2 and SnO2, in which IrO2 mainly increases the methanol oxidation activity and SnO2 mainly improves the CO oxidation ability and durability. Therefore, Pt-SnO2/IrO2/CNTs exhibits excellent performance for methanol oxidation with higher electrocatalytic activity (I(f) of 1054 A g(Pt(-1)) and powerful anti-poisoning ability (the onset potential for CO oxidation of 0.3 V) and outstanding durability (the sustained time t in CP of 617 s), revealing a suitable anode catalyst for DMFCs.

  17. Regeneration of Pt-catalysts deactivated in municipal waste flue gas with H2/N2 and the effect of regeneration step on the SCR catalyst

    DEFF Research Database (Denmark)

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

    Municipal waste flue gas was previously found to deactivate the Pt-based CO oxidation catalyst severely. In the specific case studied, siloxanes were found to cause the deactivation. An on-site method for complete regeneration of the catalyst activity was found without shutdown of the flue gas...... stream, i.e. by in situ treatment of the Pt-catalyst by reductive H2-gas. However, introduction of H2 gas in the gas stream could also affect other units in the tail pipe gas cleaning system. Of special interest here, is the effect of hydrogen gas on the performance of the deNOx + SCR catalytic process...

  18. An efficient and pH-universal ruthenium-based catalyst for the hydrogen evolution reaction

    Science.gov (United States)

    Mahmood, Javeed; Li, Feng; Jung, Sun-Min; Okyay, Mahmut Sait; Ahmad, Ishfaq; Kim, Seok-Jin; Park, Noejung; Jeong, Hu Young; Baek, Jong-Beom

    2017-05-01

    The hydrogen evolution reaction (HER) is a crucial step in electrochemical water splitting and demands an efficient, durable and cheap catalyst if it is to succeed in real applications. For an energy-efficient HER, a catalyst must be able to trigger proton reduction with minimal overpotential and have fast kinetics. The most efficient catalysts in acidic media are platinum-based, as the strength of the Pt-H bond is associated with the fastest reaction rate for the HER. The use of platinum, however, raises issues linked to cost and stability in non-acidic media. Recently, non-precious-metal-based catalysts have been reported, but these are susceptible to acid corrosion and are typically much inferior to Pt-based catalysts, exhibiting higher overpotentials and lower stability. As a cheaper alternative to platinum, ruthenium possesses a similar bond strength with hydrogen (˜65 kcal mol-1), but has never been studied as a viable alternative for a HER catalyst. Here, we report a Ru-based catalyst for the HER that can operate both in acidic and alkaline media. Our catalyst is made of Ru nanoparticles dispersed within a nitrogenated holey two-dimensional carbon structure (Ru@C2N). The Ru@C2N electrocatalyst exhibits high turnover frequencies at 25 mV (0.67 H2 s-1 in 0.5 M H2SO4 solution; 0.75 H2 s-1 in 1.0 M KOH solution) and small overpotentials at 10 mA cm-2 (13.5 mV in 0.5 M H2SO4 solution; 17.0 mV in 1.0 M KOH solution) as well as superior stability in both acidic and alkaline media. These performances are comparable to, or even better than, the Pt/C catalyst for the HER.

  19. 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.

  20. 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.

  1. Promotion of Pt-Ru/C catalysts driven by heat treated induced surface segregation for methanol oxidation reaction

    International Nuclear Information System (INIS)

    Wei Yuchen; Liu Chenwei; Chang Weijung; Wang Kuanwen

    2011-01-01

    Research highlights: → Thermal treatments on the Pt-Ru/C induce different extents of surface segregation. → O 2 treatment results in obvious Ru segregation and formation of RuO 2 . → Catalysts treated in H 2 have the excellent CO de-poisoning ability. → N 2 treatment suppresses the surface Pt depletion and hence promotes the MOR. - Abstract: Carbon supported Pt-Ru/C (1:1) alloy catalysts supplied by E-TEK are widely used for fuel cell research. Heat treatments in various atmospheres are conducted for the promotion of the methanol oxidation reaction (MOR) and the investigation of the structure-activity relationship (SAR) of the catalysts. The alloy structures, surface compositions, surface species, and electro-catalytic activities of the alloy catalysts are characterized by X-ray diffraction (XRD), temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV), respectively. The as-received Pt-Ru/C catalysts have a Ru rich in the inner core and Pt rich on the outer shell structure. Thermal treatments on the catalysts induce Ru surface segregation in different extents and thereby lead to their alteration of the alloying degrees. O 2 treatment results in obvious Ru segregation and formation of RuO 2 . Catalysts treated in H 2 have the highest I f /I b value in the CV scans among all samples, indicating the catalysts have the excellent CO de-poisoning ability as evidenced by anodic CO stripping experiments. N 2 treatment may serve as an adjustment process for the surface composition and structure of the catalysts, which can suppress the surface Pt depletion (∼60% Pt on the surface), make the components stable and hence promote the MOR significantly.

  2. Promotion of Pt-Ru/C catalysts driven by heat treated induced surface segregation for methanol oxidation reaction

    Energy Technology Data Exchange (ETDEWEB)

    Wei Yuchen; Liu Chenwei; Chang Weijung [Institute of Materials Science and Engineering, National Central University, Taoyuan 32001, Taiwan (China); Wang Kuanwen, E-mail: kuanwen.wang@gmail.com [Institute of Materials Science and Engineering, National Central University, Taoyuan 32001, Taiwan (China)

    2011-01-12

    Research highlights: > Thermal treatments on the Pt-Ru/C induce different extents of surface segregation. > O{sub 2} treatment results in obvious Ru segregation and formation of RuO{sub 2}. > Catalysts treated in H{sub 2} have the excellent CO de-poisoning ability. > N{sub 2} treatment suppresses the surface Pt depletion and hence promotes the MOR. - Abstract: Carbon supported Pt-Ru/C (1:1) alloy catalysts supplied by E-TEK are widely used for fuel cell research. Heat treatments in various atmospheres are conducted for the promotion of the methanol oxidation reaction (MOR) and the investigation of the structure-activity relationship (SAR) of the catalysts. The alloy structures, surface compositions, surface species, and electro-catalytic activities of the alloy catalysts are characterized by X-ray diffraction (XRD), temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV), respectively. The as-received Pt-Ru/C catalysts have a Ru rich in the inner core and Pt rich on the outer shell structure. Thermal treatments on the catalysts induce Ru surface segregation in different extents and thereby lead to their alteration of the alloying degrees. O{sub 2} treatment results in obvious Ru segregation and formation of RuO{sub 2}. Catalysts treated in H{sub 2} have the highest I{sub f}/I{sub b} value in the CV scans among all samples, indicating the catalysts have the excellent CO de-poisoning ability as evidenced by anodic CO stripping experiments. N{sub 2} treatment may serve as an adjustment process for the surface composition and structure of the catalysts, which can suppress the surface Pt depletion ({approx}60% Pt on the surface), make the components stable and hence promote the MOR significantly.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-03-30

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

  4. 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.

  5. Pt Single Atoms Embedded in the Surface of Ni Nanocrystals as Highly Active Catalysts for Selective Hydrogenation of Nitro Compounds.

    Science.gov (United States)

    Peng, Yuhan; Geng, Zhigang; Zhao, Songtao; Wang, Liangbing; Li, Hongliang; Wang, Xu; Zheng, Xusheng; Zhu, Junfa; Li, Zhenyu; Si, Rui; Zeng, Jie

    2018-06-13

    Single-atom catalysts exhibit high selectivity in hydrogenation due to their isolated active sites, which ensure uniform adsorption configurations of substrate molecules. Compared with the achievement in catalytic selectivity, there is still a long way to go in exploiting the catalytic activity of single-atom catalysts. Herein, we developed highly active and selective catalysts in selective hydrogenation by embedding Pt single atoms in the surface of Ni nanocrystals (denoted as Pt 1 /Ni nanocrystals). During the hydrogenation of 3-nitrostyrene, the TOF numbers based on surface Pt atoms of Pt 1 /Ni nanocrystals reached ∼1800 h -1 under 3 atm of H 2 at 40 °C, much higher than that of Pt single atoms supported on active carbon, TiO 2 , SiO 2 , and ZSM-5. Mechanistic studies reveal that the remarkable activity of Pt 1 /Ni nanocrystals derived from sufficient hydrogen supply because of spontaneous dissociation of H 2 on both Pt and Ni atoms as well as facile diffusion of H atoms on Pt 1 /Ni nanocrystals. Moreover, the ensemble composed of the Pt single atom and nearby Ni atoms in Pt 1 /Ni nanocrystals leads to the adsorption configuration of 3-nitrostyrene favorable for the activation of nitro groups, accounting for the high selectivity for 3-vinylaniline.

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

    Science.gov (United States)

    Hassan, Ayaz; Ticianelli, Edson A

    2018-01-01

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

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

    Directory of Open Access Journals (Sweden)

    AYAZ HASSAN

    2018-04-01

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

  8. Engineering Ru@Pt Core-Shell Catalysts for Enhanced Electrochemical Oxygen Reduction Mass Activity and Stability

    Directory of Open Access Journals (Sweden)

    Ariel Jackson

    2018-01-01

    Full Text Available Improving the performance of oxygen reduction reaction (ORR electrocatalysts is essential for the commercial efficacy of many renewable energy technologies, including low temperature polymer electrolyte fuel cells (PEFCs. Herein, we report highly active and stable carbon-supported Ru@Pt core-shell nanoparticles (Ru@Pt/C prepared by a wet chemical synthesis technique. Through rotating disc electrode testing, the Ru@Pt/C achieves an ORR Pt mass-based activity of 0.50 A mgPt−1 at 0.9 V versus the reversible hydrogen electrode (RHE, which exceeds the activity of the state-of-the-art commercial Pt/C catalyst as well as the Department of Energy 2020 PEFC electrocatalyst activity targets for transportation applications. The impact of various synthetic parameters, including Pt to Ru ratios and catalyst pretreatments (i.e., annealing are thoroughly explored. Pt-based mass activity of all prepared Ru@Pt/C catalysts was found to exceed 0.4 mgPt−1 across the range of compositions investigated, with the maximum activity catalyst having a Ru:Pt ratio of 1:1. This optimized composition of Ru@Pt/C catalyst demonstrated remarkable stability after 30,000 accelerated durability cycles (0.6 to 1.0 V vs. RHE at 125 mV s−1, maintaining 85% of its initial mass activity. Scanning transmission electron microscopy energy dispersive spectroscopy (STEM-EDS analysis at various stages of electrochemical testing demonstrated that the Pt shell can provide sufficient protection against the dissolution of the otherwise unstable Ru core.

  9. TiO2 and Al2O3 promoted Pt/C nanocomposites as low temperature fuel cell catalysts for electro oxidation of methanol in acidic media

    International Nuclear Information System (INIS)

    Naeem, Rabia; Ahmed, Riaz; Ansari, Muhammad Shahid

    2014-01-01

    Carbon corrosion and platinum dissolution are the two major catalyst layer degradation problems in polymer electrolyte membrane fuel cells (PEMFC). Ceramic addition can reduce the corrosion of carbon and increase the stability of catalysts. Pt/TiO 2 , Pt/TiO 2 -C, Pt/Al 2 O 3 and Pt/Al 2 O 3 -C catalysts were synthesized and characterized. Electrochemical surface area of Pt/TiO 2 -C and Pt/Al 2 O 3 -C nanocomposite catalysts was much higher than the Pt/TiO 2 and Pt/Al 2 O 3 catalysts. Peak current, specific activity and mass activity of the catalysts was also determined by cyclic voltammetry and were much higher for the carbon nanocomposites. Exchange current densities were determined from Tafel plots. Heterogeneous rates of reaction of electro oxidation of methanol were determined for all the catalysts and were substantially higher for titania catalysts as compared to alumina added catalysts. Mass activity of Pt/TiO 2 -C was much higher than mass activity of Pt/Al 2 O 3 -C. Stability studies showed that addition of ceramics have increased the catalytic activity and durability of the catalysts considerably

  10. Pt-Rh/g Al2O3 Influence of Catalyst Preparation Methods on Metallic Particle Dispersion and Size Distribution

    Directory of Open Access Journals (Sweden)

    N.M. da Fonseca

    1998-06-01

    Full Text Available - Pt-Rh/Al2O3 catalysts were prepared by successive incipient impregnations or coimpregnation. Characterization was achieved by H2 chemisorption and transmission electron microscopy. It was verified that method of preparation, ratio of metal weights and sequence of deposition are factors that result in very distinct catalysts.

  11. Highly selective bimetallic Pt-Cu/Mg(Al)O catalysts for the aqueous-phase reforming of glycerol

    NARCIS (Netherlands)

    Boga, D.A.; Oord, R.; Beale, A.M.; Chung, Y.M.; Bruijnincx, P.C.A.; Weckhuysen, B.M.

    2013-01-01

    Monometallic Pt and bimetallic Pt-Cu catalysts supported on Mg(Al)O mixed oxides, obtained by calcination of the corresponding layered double hydroxides (LDHs), were prepared and tested in the aqueous-phase reforming (APR) of glycerol. The effect of the Mg/Al ratio and calcination temperature of the

  12. Exploring the Potential of Different-Sized Supported Subnanometer Pt Clusters as Catalysts for Wet Chemical Applications

    KAUST Repository

    Rondelli, Manuel; Zwaschka, Gregor; Krause, Maximilian; Rö tzer, Marian D.; Hedhili, Mohamed N.; Hogerl, Manuel Peter; D’ Elia, Valerio; Schweinberger, Florian F.; Basset, Jean-Marie; Heiz, Ueli

    2017-01-01

    as catalysts for organic chemistry transformations in solution has not been explored. To this end, single Pt atoms and Pt clusters with two narrow size distributions were prepared in the UHV and applied for the hydrogenation of p-chloronitrobenzene to p

  13. Calcined eggshell (CES): An efficient natural catalyst for ...

    Indian Academy of Sciences (India)

    hydes with active methylene compounds using calcined eggshell (CES) as an efficient ... of the important reactions to achieve carbon–carbon ... solid catalyst for biodiesel production,24 as a catalyst ... which supports for adsorption of water on CaO and ... The organic phase .... After extraction of the product with ethylac-.

  14. An extraordinarily stable catalyst: Pt NPs supported on two-dimensional Ti3C2X2 (X = OH, F) nanosheets for oxygen reduction reaction.

    Science.gov (United States)

    Xie, Xiaohong; Chen, Siguo; Ding, Wei; Nie, Yao; Wei, Zidong

    2013-10-03

    High dispersion Pt nanoparticles supported on 2D Ti3C2X2 (X = OH, F) nanosheets are presented and electro-chemical measurements confirm that the Pt/Ti3C2X2 catalyst shows enhanced durability and improved ORR activity compared with the commercial Pt/C catalyst.

  15. Structure–activity relationships of Pt/Al2O3 catalysts for CO and NO oxidation at diesel exhaust conditions

    DEFF Research Database (Denmark)

    Boubnov, Alexey; Dahl, Søren; Johnson, Erik

    2012-01-01

    Structure–performance relationships for Pt/Al2O3 catalysts with mean Pt particle sizes of 1, 2, 3, 5 and 10nm are investigated for the catalytic oxidation of CO and NO under lean-burning diesel exhaust conditions. The most active catalysts for CO oxidation exhibit Pt particles of 2–3nm, having...

  16. Towards Highly Performing and Stable PtNi Catalysts in Polymer Electrolyte Fuel Cells for Automotive Application

    Directory of Open Access Journals (Sweden)

    Sabrina C. Zignani

    2017-03-01

    Full Text Available In order to help the introduction on the automotive market of polymer electrolyte fuel cells (PEFCs, it is mandatory to develop highly performing and stable catalysts. The main objective of this work is to investigate PtNi/C catalysts in a PEFC under low relative humidity and pressure conditions, more representative of automotive applications. Carbon supported PtNi nanoparticles were prepared by reduction of metal precursors with formic acid and successive thermal and leaching treatments. The effect of the chemical composition, structure and surface characteristics of the synthesized samples on their electrochemical behavior was investigated. The catalyst characterized by a larger Pt content (Pt3Ni2/C presented the highest catalytic activity (lower potential losses in the activation region among the synthesized bimetallic PtNi catalysts and the commercial Pt/C, used as the reference material, after testing at high temperature (95 °C and low humidification (50% conditions for automotive applications, showing a cell potential (ohmic drop-free of 0.82 V at 500 mA·cm−2. In order to assess the electro-catalysts stability, accelerated degradation tests were carried out by cycling the cell potential between 0.6 V and 1.2 V. By comparing the electrochemical and physico-chemical parameters at the beginning of life (BoL and end of life (EoL, it was demonstrated that the Pt1Ni1/C catalyst was the most stable among the catalyst series, with only a 2% loss of voltage at 200 mA·cm−2 and 12.5% at 950 mA·cm−2. However, further improvements are needed to produce durable catalysts.

  17. Surface composition of magnetron sputtered Pt-Co thin film catalyst for proton exchange membrane fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Vorokhta, Mykhailo, E-mail: vorohtam@gmail.com [Charles University in Prague, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holešovičkách 2, 18000 Prague (Czech Republic); Khalakhan, Ivan; Václavů, Michal [Charles University in Prague, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holešovičkách 2, 18000 Prague (Czech Republic); Kovács, Gábor; Kozlov, Sergey M. [Departament de Química Física and Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, c/ Martí i Franquès 1, 08028 Barcelona (Spain); Kúš, Peter; Skála, Tomáš; Tsud, Natalia; Lavková, Jaroslava [Charles University in Prague, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holešovičkách 2, 18000 Prague (Czech Republic); Potin, Valerie [Laboratoire Interdisciplinaire Carnot de Bourgogne, UMR 6303 CNRS-Université Bourgogne, 9 Av. A. Savary, BP 47870, F-21078 Dijon Cedex (France); and others

    2016-03-01

    Graphical abstract: - Highlights: • Nanostructured Pt-Co thin catalyst films were grown on carbon by magnetron sputtering. • The surface composition of the nanostructured Pt-Co films was investigated by surface analysis techniques. • We carried out modeling of Pt-Co nanoalloys by computational methods. • Both experiment and modeling based on density functional theory showed that the surface of Pt-Co nanoparticles is almost exclusively composed of Pt atoms. - Abstract: Recently we have tested a magnetron sputtered Pt-Co catalyst in a hydrogen-fed proton exchange membrane fuel cell and showed its high catalytic activity for the oxygen reduction reaction. Here we present further investigation of the magnetron sputtered Pt-Co thin film catalyst by both experimental and theoretical methods. Scanning electron microscopy and transmission electron microscopy experiments confirmed the nanostructured character of the catalyst. The surface composition of as-deposited and annealed at 773 K Pt-Co films was investigated by surface analysis techniques, such as synchrotron radiation photoelectron spectroscopy and X-ray photoelectron spectroscopy. Modeling based on density functional theory showed that the surface of 6 nm large 1:1 Pt-Co nanoparticles is almost exclusively composed of Pt atoms (>90%) at typical operation conditions and the Co content does not exceed 20% at 773 K, in agreement with the experimental characterization of such films annealed in vacuum. According to experiment, the density of valence states of surface atoms in Pt-Co nanostructures is shifted by 0.3 eV to higher energies, which can be associated with their higher activity in the oxygen reduction reaction. The changes in electronic structure caused by alloying are also reflected in the measured Pt 4f, Co 3p and Co 2p photoelectron peak binding energies.

  18. Dehydrogenation of Light Alkanes over Supported Pt Catalysts

    OpenAIRE

    Wu, Jason

    2015-01-01

    The production of light alkenes comprises a 250 million ton per year industry due to their extensive use in the production of plastics, rubbers, fuel blending agents, and chemical intermediates. While steam cracking and fluid catalytic cracking of petroleum crude oils are the most common methods for obtaining light alkenes, rising oil prices and low selectivities toward specific alkenes have driven the search for a more economical and efficient process. Catalytic dehydrogenation of light alka...

  19. High-temperature catalytic reforming of n-hexane over supported and core-shell Pt nanoparticle catalysts: role of oxide-metal interface and thermal stability.

    Science.gov (United States)

    An, Kwangjin; Zhang, Qiao; Alayoglu, Selim; Musselwhite, Nathan; Shin, Jae-Youn; Somorjai, Gabor A

    2014-08-13

    Designing catalysts with high thermal stability and resistance to deactivation while simultaneously maintaining their catalytic activity and selectivity is of key importance in high-temperature reforming reactions. We prepared Pt nanoparticle catalysts supported on either mesoporous SiO2 or TiO2. Sandwich-type Pt core@shell catalysts (SiO2@Pt@SiO2 and SiO2@Pt@TiO2) were also synthesized from Pt nanoparticles deposited on SiO2 spheres, which were encapsulated by either mesoporous SiO2 or TiO2 shells. n-Hexane reforming was carried out over these four catalysts at 240-500 °C with a hexane/H2 ratio of 1:5 to investigate thermal stability and the role of the support. For the production of high-octane gasoline, branched C6 isomers are more highly desired than other cyclic, aromatic, and cracking products. Over Pt/TiO2 catalyst, production of 2-methylpentane and 3-methylpentane via isomerization was increased selectively up to 420 °C by charge transfer at Pt-TiO2 interfaces, as compared to Pt/SiO2. When thermal stability was compared between supported catalysts and sandwich-type core@shell catalysts, the Pt/SiO2 catalyst suffered sintering above 400 °C, whereas the SiO2@Pt@SiO2 catalyst preserved the Pt nanoparticle size and shape up to 500 °C. The SiO2@Pt@TiO2 catalyst led to Pt nanoparticle sintering due to incomplete protection of the TiO2 shells during the reaction at 500 °C. Interestingly, over the Pt/TiO2 catalyst, the average size of Pt nanoparticles was maintained even after 500 °C without sintering. In situ ambient pressure X-ray photoelectron spectroscopy demonstrated that the Pt/TiO2 catalyst did not exhibit TiO2 overgrowth on the Pt surface or deactivation by Pt sintering up to 600 °C. The extraordinarily high stability of the Pt/TiO2 catalyst promoted high reaction rates (2.0 μmol · g(-1) · s(-1)), which was 8 times greater than other catalysts and high isomer selectivity (53.0% of C6 isomers at 440 °C). By the strong metal-support interaction

  20. Synthesis and Electrochemical Evaluation of Carbon Supported Pt-Co Bimetallic Catalysts Prepared by Electroless Deposition and Modified Charge Enhanced Dry Impregnation

    Directory of Open Access Journals (Sweden)

    John Meynard M. Tengco

    2016-06-01

    Full Text Available Carbon-supported bimetallic Pt-Co cathode catalysts have been previously identified as higher activity alternatives to conventional Pt/C catalysts for fuel cells. In this work, a series of Pt-Co/C catalysts were synthesized using electroless deposition (ED of Pt on a Co/C catalyst prepared by modified charge enhanced dry impregnation. X-ray diffraction (XRD and scanning transmission electron microscopy (STEM characterization of the base catalyst showed highly dispersed particles. A basic ED bath containing PtCl62− as the Pt precursor, dimethylamine borane as reducing agent, and ethylenediamine as stabilizing agent successfully targeted deposition of Pt on Co particles. Simultaneous action of galvanic displacement and ED resulted in Pt-Co alloy formation observed in XRD and energy dispersive X-ray spectroscopy (XEDS mapping. In addition, fast deposition kinetics resulted in hollow shell Pt-Co alloy particles while particles with Pt-rich shell and Co-rich cores formed with controlled Pt deposition. Electrochemical evaluation of the Pt-Co/C catalysts showed lower active surface but much higher mass and surface activities for oxygen reduction reaction compared to a commercial Pt/C fuel cell catalyst.

  1. Engineering Pt/Pd Interfacial Electronic Structures for Highly Efficient Hydrogen Evolution and Alcohol Oxidation.

    Science.gov (United States)

    Fan, Jinchang; Qi, Kun; Zhang, Lei; Zhang, Haiyan; Yu, Shansheng; Cui, Xiaoqiang

    2017-05-31

    Tailoring the interfacial structure of Pt-based catalysts has emerged as an effective strategy to improve catalytic activity. However, little attention has been focused on investigating the relationship between the interfacial facets and their catalytic activity. Here, we design and implement Pd-Pt interfaces with controlled heterostructure features by epitaxially growing Pt nanoparticles on Pd nanosheets. On the basis of both density functional theory calculation and experimental results, we demonstrate that charge transfer from Pd to Pt is highly dependent on the interfacial facets of Pd substrates. Therefore, the Pd-Pt heterostructure with Pd(100)-Pt interface exhibits excellent activity and long-term stability for hydrogen evolution and methanol/ethanol oxidation reactions in alkaline medium, much better than that with Pd (111)-Pt interface or commercial Pt/C. Interfacial crystal facet-dependent electronic structural modulation sheds a light on the design and investigation of new heterostructures for high-activity catalysts.

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

    International Nuclear Information System (INIS)

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

    2009-01-01

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

  3. PtRu catalysts supported on heteropolyacid and chitosan functionalized carbon nanotubes for methanol oxidation reaction of fuel cells.

    Science.gov (United States)

    Cui, Zhiming; Li, Chang Ming; Jiang, San Ping

    2011-09-28

    A simple self-assembly approach has been developed to functionalize carbon nanotubes (CNTs) with chitosan (CS) and heteropolyacids (HPAs) of phosphomolybdic acid (H(3)PMo(12)O(40), HPMo) and phosphotungstic acid (H(3)PW(12)O(40), HPW). The non-covalent functionalization method, which introduces homogenous surface functional groups with no detrimental effect on graphene structures of CNTs, can be carried out at room temperature without the use of corrosive acids. The PtRu nanoparticles supported on HPAs-CS-CNTs have a uniform distribution and much smaller size as compared to those of the PtRu nanoparticles supported on conventional acid treated CNTs (PtRu/AO-CNTs). The onset and peak potentials for CO(ad) oxidation on PtRu/HPAs-CS-CNTs catalysts are more negative than those on PtRu/AO-CNTs, indicating that HPAs facilitate the electro-oxidation of CO. The PtRu/HPMo-CS-CNTs catalyst has a higher electrocatalytic activity for methanol oxidation and higher tolerance toward CO poisoning than PtRu/HPW-CS-CNTs. The better electrocatalytic enhancement of HPMo on the PtRu/HPAs-CS-CNTs catalyst is most likely related to the fact that molybdenum-containing HPAs such as HPMo have more labile terminal oxygen to provide additional active oxygen sites while accelerating the CO and methanol oxidation in a similar way to that of Ru in the PtRu binary alloy system.

  4. Applications of hydrophobic Pt catalysts in separation of tritium from liquid effluents

    International Nuclear Information System (INIS)

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

    2003-01-01

    Hydrophobic Pt catalysts were first prepared and used in deuterium or tritium separation while after their application was extended to chemical reactions occurring in liquid water or saturated humidity environments. Capillary condensing produced at the contact with liquid water or vapors engenders in classical hydrophilic catalysts a decrease in activity what makes them inefficient. Consequently, liquid water 'repealing' catalysts are to be used allowing, at the same time gaseous reactants and reaction products to diffuse to and fro the catalytic active centers. These catalysts were successfully applied in deuterium enrichment and tritium separation based on hydrogen- liquid water isotopic exchange at both pilot and industrial scale. High activity and a prolonged stability were demonstrated and checked in: - detritiation of the heavy water used as both moderator and coolant in CANDU type reactors; removing of tritium from light water recirculated in nuclear fuel reprocessing facilities; removal and recovery of tritium from atmosphere and tritium processing installations. Due to their incontestable advantages the use of these catalysts was recently extended to other chemical processes occurring in the presence of liquid water or in high humidity environment or else when water occurs as a reaction product, such as catalytic hydrogen - oxygen recombination at room temperature or removal of stable organic pollutants from waste waters

  5. Catalysts Efficiency Evaluation by using CC Analysis Test

    Directory of Open Access Journals (Sweden)

    Arina Negoitescu

    2011-10-01

    Full Text Available The study emphasizes the necessity of the catalysts efficiency testing. Diagnosis systems using lambda probes are based on the capacity of the catalyst oxygen storage. Comparing the lambda probe signals upstream and downstream of catalyst provides an indication on catalyst activity, although the correlation between oxygen storage capacity and catalyst efficiency is still difficult. Diagnosis for the 1.4 Renault Clio Symbol was accomplished in the Road Vehicles Lab at the Politehnica University of Timisoara using AVL Dicom 4000. The tests showed that the engine worked with lean mixture being necessary a fuel mixture correction calculated by the control unit ECU. A compensation of 0.14 % vol is required for the engine correct operation and emissions integration within permissible limits

  6. Platinum(0-1,3-divinyl-1,1,3,3-tetramethyldisiloxane Complex as a Pt Source for Pt/SnO2 Catalyst

    Directory of Open Access Journals (Sweden)

    Agnieszka Martyla

    2014-01-01

    Full Text Available This paper presents new preparation method of Pt/SnO2, an important catalytic system. Besides of its application as a heterogenic industrial catalyst, it is also used as a catalyst in electrochemical processes, especially in fuel cells. Platinum is commonly used as an anode catalyst in low temperature fuel cells, fuelled with alcohols of low molecular weight such as methanol. Platinum(0-1,3-divinyl-1,1,3,3-tetramethyldisiloxane complex was used as a precursor of metallic phase. The aim of the research was to obtain a highly active in electrochemical system Pt/SnO2 catalyst with low metal load. Considering small size of Pt crystallites, it should result in high activity of Pt/SnO2 system. The presented method of SnO2 synthesis allows for obtaining support consisting of nanoparticles. The effect of the thermal treatment on activity of Pt/SnO2 gel was demonstrated. The system properties were investigated using TEM, FTIR (ATR, and XRD techniques to describe its thermal structural evolution. The results showed two electrocatalytical activity peaks for drying at a temperature of 430 K and above 650 K.

  7. Pt/XC-72 catalysts coated with nitrogen-doped carbon (Pt/XC-72@C–N) for methanol electro-oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Cao, Jun; Chu, Yuanyuan; Tan, Xiaoyao, E-mail: cestanxy@aliyun.com

    2014-03-01

    Pt/XC-72 catalysts coated with N-doped carbon (denoted as Pt/XC-72@C–N) for the electro-oxidation of methanol are prepared through a combined microwave-assisted polyol with in-situ carbonization of N-doped carbon coating process using polyvinylpyrrolidone (PVP), 1-vinyl-3-ethylimidazolium nitrate (VEIN) or 1-ethyl-3-methylimidazolium dicyanamide (EMID) ionic liquid as the N-doped carbon precursor. X-ray diffraction, energy dispersive of X-ray, transmission electron microscopy, X-ray photoelectron spectroscopy, cyclic voltammograms and accelerated aging test techniques are applied to characterize the structure and the electro-catalytic activity of the catalysts. The results show that the Pt particles with the average size of around 2.5 nm are highly dispersed in face-centered cubic crystal structure in the carbon support. The structure of the N-doped carbon coating precursor has considerable influence on the electro-catalytic performance of the catalysts. The resultant catalyst with EMID ionic liquid as the N-doped carbon source exhibits 115.9 m{sup 2} g{sup −1}Pt electrochemical surface area (ESA) and 0.66 A mg{sup −1}Pt catalytic activity towards the electro-oxidation of methanol, which are 1.37 times the ESA and 1.35 times the catalytic activity of the PVP-derived catalyst, and 2.02 times the electrochemical surface area and 1.94 times the catalytic activity of the VEIN-derived catalyst. The appropriate amount of the EMID ionic liquid used in the catalyst synthesis process is around 10 uL for 100 mg XC-72 support so as to obtain the highest electro-catalytic activity. - Highlights: • N-doped carbon coated Pt/C catalyst is prepared for methanol electro-oxidation. • Pt/XC-72@C–N exhibits excellent electrocatalytic activity over uncoated catalysts. • Ionic liquid with anionic cyano groups is most suitable as N-doped carbon precursor. • The appropriate amount of ionic liquid for coating is around 10 μL for 100 mg carbon.

  8. Methods to synthesize NiPt bimetallic nanoparticles by a reversed-phase microemulsion, deposition of NiPt bimetallic nanoparticles on a support, and application of the supported catalyst for CO.sub.2 reforming of methane

    KAUST Repository

    Biausque, Gregory; Laveille, Paco; Anjum, Dalaver H.; Caps, Valerie; Basset, Jean-Marie

    2015-01-01

    Methods to synthesize NiPt bimetallic nanoparticles by a reversed-phase microemulsion, deposition of NiPt bimetallic nanoparticles on a support, and application of the supported catalyst for CO.sub.2 reforming of methane

  9. Methods to synthesize NiPt bimetallic nanoparticles by a reversed-phase microemulsion, deposition of NiPt bimetallic nanoparticles on a support, and application of the supported catalyst for CO.sub.2 reforming of methane

    KAUST Repository

    Biausque, Gregory

    2015-04-28

    Methods to synthesize NiPt bimetallic nanoparticles by a reversed-phase microemulsion, deposition of NiPt bimetallic nanoparticles on a support, and application of the supported catalyst for CO.sub.2 reforming of methane

  10. Synthesis of Fe3O4/Pt Nanoparticles Decorated Carbon Nanotubes and Their Use as Magnetically Recyclable Catalysts

    Directory of Open Access Journals (Sweden)

    Hongkun He

    2011-01-01

    Full Text Available We report a facile approach to prepare Fe3O4/Pt nanoparticles decorated carbon nanotubes (CNTs. The superparamagnetic Fe3O4 nanoparticles with average size of 4∼5 nm were loaded on the surfaces of carboxyl groups functionalized CNTs via a high-temperature solution-phase hydrolysis method from the raw material of FeCl3. The synthesis process of magnetic CNTs is green and readily scalable. The loading amounts of Fe3O4 nanopartilces and the magnetizations of the resulting magnetic CNTs show good tunability. The Pt nanopaticles with average size of 2.5 nm were deposited on the magnetic CNTs through a solution-based method. It is demonstrated that the Fe3O4/Pt nanoparticles decorated CNTs have high catalytic activity in the reduction reaction of 4-nitrophenol and can be readily recycled by a magnet and reused in the next reactions with high efficiencies for at least fifteen successive cycles. The novel CNTs-supported magnetically recyclable catalysts are promising in heterogeneous catalysis applications.

  11. Synthesis of Fe3O4/Pt Nanoparticles Decorated Carbon Nano tubes and Their Use as Magnetically Recyclable Catalysts

    International Nuclear Information System (INIS)

    He, H.; Gao, C.

    2011-01-01

    We report a facile approach to prepare Fe 3 O 4 /Pt nanoparticles decorated carbon nano tubes (CNTs). The superparamagnetic Fe 3 O 4 nanoparticles with average size of 45 nm were loaded on the surfaces of carboxyl groups functionalized CNTs via a high-temperature solution-phase hydrolysis method from the raw material of FeCl 3 . The synthesis process of magnetic CNTs is green and readily scalable. The loading amounts of Fe 3 O 4 nanoparticles and the magnetizations of the resulting magnetic CNTs show good tunability. The Pt nanoparticles with average size of 2.5 nm were deposited on the magnetic CNTs through a solution-based method. It is demonstrated that the Fe 3 O 4 /Pt nanoparticles decorated CNTs have high catalytic activity in the reduction reaction of 4-nitrophenol and can be readily recycled by a magnet and reused in the next reactions with high efficiencies for at least fifteen successive cycles. The novel CNTs-supported magnetically recyclable catalysts are promising in heterogeneous catalysis applications.

  12. Durability Improvement of Pt/RGO Catalysts for PEMFC by Low-Temperature Self-Catalyzed Reduction.

    Science.gov (United States)

    Sun, Kang Gyu; Chung, Jin Suk; Hur, Seung Hyun

    2015-12-01

    Pt/C catalyst used for polymer electrolyte membrane fuel cells (PEMFCs) displays excellent initial performance, but it does not last long because of the lack of durability. In this study, a Pt/reduced graphene oxide (RGO) catalyst was synthesized by the polyol method using ethylene glycol (EG) as the reducing agent, and then low-temperature hydrogen bubbling (LTHB) treatment was introduced to enhance the durability of the Pt/RGO catalyst. The cyclic voltammetry (CV), oxygen reduction reaction (ORR) analysis, and transmittance electron microscopy (TEM) results suggested that the loss of the oxygen functional groups, because of the hydrogen spillover and self-catalyzed dehydration reaction during LTHB, reduced the carbon corrosion and Pt agglomeration and thus enhanced the durability of the electrocatalyst.

  13. Dry (CO_2) reforming of methane over Pt catalysts studied by DFT and kinetic modeling

    International Nuclear Information System (INIS)

    Niu, Juntian; Du, Xuesen; Ran, Jingyu; Wang, Ruirui

    2016-01-01

    Graphical abstract: - Highlights: • CH appears to be the most abundant species on Pt(1 1 1) surface in CH_4 dissociation. • CO_2* + H* → COOH* + * → CO* + OH* is the dominant reaction pathway in CO_2 activation. • Major reaction pathway in CH oxidation: CH* + OH* → CHOH* + * → CHO* + H* → CO* + 2H*. • C* + OH* → COH* + * → CO* + H* is the dominant reaction pathway in C oxidation. - Abstract: Dry reforming of methane (DRM) is a well-studied reaction that is of both scientific and industrial importance. In order to design catalysts that minimize the deactivation and improve the selectivity and activity for a high H_2/CO yield, it is necessary to understand the elementary reaction steps involved in activation and conversion of CO_2 and CH_4. In our present work, a microkinetic model based on density functional theory (DFT) calculations is applied to explore the reaction mechanism for methane dry reforming on Pt catalysts. The adsorption energies of the reactants, intermediates and products, and the activation barriers for the elementary reactions involved in the DRM process are calculated over the Pt(1 1 1) surface. In the process of CH_4 direct dissociation, the kinetic results show that CH dissociative adsorption on Pt(1 1 1) surface is the rate-determining step. CH appears to be the most abundant species on the Pt(1 1 1) surface, suggesting that carbon deposition is not easy to form in CH_4 dehydrogenation on Pt(1 1 1) surface. In the process of CO_2 activation, three possible reaction pathways are considered to contribute to the CO_2 decomposition: (I) CO_2* + * → CO* + O*; (II) CO_2* + H* → COOH* + * → CO* + OH*; (III) CO_2* + H* → mono-HCOO* + * → bi-HCOO* + * [CO_2* + H* → bi-HCOO* + *] → CHO* + O*. Path I requires process to overcome the activation barrier of 1.809 eV and the forward reaction is calculated to be strongly endothermic by 1.430 eV. In addition, the kinetic results also indicate this process is not easy to

  14. 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.

  15. Real-Time Optical Monitoring of Pt Catalyst Under the Potentiodynamic Conditions

    Science.gov (United States)

    Song, Hyeon Don; Lee, Minzae; Kim, Gil-Pyo; Choi, Inhee; Yi, Jongheop

    2016-12-01

    In situ monitoring of electrode materials reveals detailed physicochemical transition in electrochemical device. The key challenge is to explore the localized features of electrode surfaces, since the performance of an electrochemical device is determined by the summation of local architecture of the electrode material. Adaptive in situ techniques have been developed for numerous investigations; however, they require restricted measurement environments and provide limited information, which has impeded their widespread application. In this study, we realised an optics-based electrochemical in situ monitoring system by combining a dark-field micro/spectroscopy with an electrochemical workstation to investigate the physicochemical behaviours of Pt catalyst. We found that the localized plasmonic trait of a Pt-decorated Au nanoparticle as a model system varied in terms of its intensity and wavelength during the iterations of a cyclic voltammetry test. Furthermore, we show that morphological and compositional changes of the Pt catalyst can be traced in real time using changes in quantified plasmonic characteristics, which is a distinct advantage over the conventional electrochemistry-based in situ monitoring systems. These results indicate the substantial promise of online operando observation in a wide range of electrical energy conversion systems and electrochemical sensing areas.

  16. Catalytic Hydrodeoxygenation of Bio-oil Model Compounds over Pt/HY Catalyst

    Science.gov (United States)

    Lee, Heejin; Kim, Hannah; Yu, Mi Jin; Ko, Chang Hyun; Jeon, Jong-Ki; Jae, Jungho; Park, Sung Hoon; Jung, Sang-Chul; Park, Young-Kwon

    2016-06-01

    The hydrodeoxygenation of a model compound of lignin-derived bio-oil, guaiacol, which can be obtained from the pyrolysis of biomass to bio-oil, has attracted considerable research attention because of its huge potential as a substitute for conventional fuels. In this study, platinum-loaded HY zeolites (Pt/HY) with different Si/Al molar ratios were used as catalysts for the hydrodeoxygenation of guaiacol, anisole, veratrole, and phenol to a range of hydrocarbons, such as cyclohexane. The cyclohexane (major product) yield increased with increasing number of acid sites. To produce bio-oil with the maximum level of cyclohexane and alkylated cyclohexanes, which would be suitable as a substitute for conventional transportation fuels, the Si/Al molar ratio should be optimized to balance the Pt particle-induced hydrogenation with acid site-induced methyl group transfer. The fuel properties of real bio-oil derived from the fast pyrolysis of cork oak was improved using the Pt/HY catalyst.

  17. Preparation for Pt-Loaded Zeolite Catalysts Using w/o Microemulsion and Their Hydrocracking Behaviors on Fischer-Tropsch Product

    Directory of Open Access Journals (Sweden)

    Toshiaki Hanaoka

    2015-02-01

    Full Text Available Pt-loaded β-type zeolite catalysts with constant Pt content (0.11 wt.% and similar pore structure were prepared using a water-in-oil (w/o microemulsion. The effect of Pt particle synthesis conditions using microemulsion (a type of Pt complex-forming agents and the molar ratio of complex-forming agent to Pt4+ on loaded Pt particle size was investigated. The Pt particle size of the Pt catalyst using tetraethylammonium chloride (TEAC as a complex-forming agent with the molar TEAC/Pt ratio 10 was the minimum value (3.8 nm, and was much smaller than that (6.7 nm prepared by the impregnation method. The utilization of the complex-forming agent of which hydrophobic groups occupied a small volume and the appropriate complex-forming agent/Pt ratio were favorable for synthesis of small Pt particles. The effect of loaded Pt particle size on the hydrocracking of the Fischer-Tropsch (FT product was investigated using the Pt-loaded zeolite catalysts at 250 °C with an initial H2 pressure of 0.5 MPa, and reaction time of 1 h. The Pt catalyst with a Pt particle size of 4.2 nm prepared using the microemulsion exhibited the maximum corresponding jet fuel yield (30.0%, which was higher than that of the impregnated catalyst.

  18. Unsupported NiPt alloy metal catalysts prepared by water-in-oil (W/O) microemulsion method for methane cracking

    KAUST Repository

    Zhou, Lu

    2016-05-18

    Unsupported NiPt metal catalyst with Ni/Pt molar ratio of 88/12 is prepared by water-in-oil (W/O) microemulsion method in this study. Compared to monometallic Ni and Pt catalysts, the NiPt catalyst exhibits superior activity and stability for methane cracking. By XRD (X-ray powder diffraction), XPS (X-ray photoelectron spectroscopy) and TEM (Transmission electron microscopy) analyses, the formation of Ni(0)Pt(0) alloy is believed to be the main reason for the reactivity improvement of this catalyst. Carbon nano tube (CNT) with Ni(0)Pt(0) particles anchored on the top of tube are found for the NiPt catalyst. © 2016 Elsevier Ltd.

  19. Propylene oxidation on catalytic Pt-Cu/y alumina. (Part II) chemical Kinetics of catalysts of Pt-Cu/y-alumina in the propylene oxidation

    International Nuclear Information System (INIS)

    Carballo, Luis M; Zea, Hugo R

    1999-01-01

    In this work is treated the effect of the composition of catalysts of Pt-Cu/y - alumina on the specific superficial activity corresponding to the total oxidation of propylene. Although the catalyst activity of the Cu in the operation conditions went practically null the specific activity of the catalytic Pt-Cu it incremented with the increase of the contained proportion of Cu in the catalyst. The total global speed by gram of catalyst was also increased with the introduction of Cu, but only to medium and high concentrations of propylene. The specific superficial activity was bigger for the sinterizated catalyst, for a given composition of the bimetallic catalyst, compared with that of the fresh catalyst (non-sinterizated). To explain, the catalytic behavior of the propylene oxidation, on the catalysts here studied, it is postulated that the propylene molecule it absorb with less force on the faces than in the corners or borders of the crystals of the catalyst and that the connection of adsorption on a place of given Pt is affected by the atoms of neighboring Cu on the surface causing changes in the mobility of the absorbed species. The kinetic results reveal a complex dependence between the reaction speed and the concentration of the propylene. In low concentrations of propylene the reaction speed was increased until to reach a maximum, and then to continue with a marked decreasing; and to concentrations. In bigger propylene concentrations, the reaction kinetics is presented as zero order with regard to the propylene, for some given concentrations of oxygen

  20. PtRu nanoparticles dispersed on nitrogen-doped carbon nanohorns as an efficient electrocatalyst for methanol oxidation reaction

    International Nuclear Information System (INIS)

    Zhang, Linwei; Gao, Ang; Liu, Yan; Wang, Yuan; Ma, Jiantai

    2014-01-01

    Highlights: • A novel anode catalyst is synthesized using N-doped carbon nanohorns as support. • PtRu/NCNHs exhibits an excellent activity for MOR relative to PtRu/C catalysts. • The enhancement is due to the electronic interaction between NCNHs and PtRu NPs. - Abstract: A novel anode catalyst (PtRu/NCNHs) assembled with nitrogen-doped carbon nanohorns (NCNHs) and PtRu nanoparticles (1.9 nm) exhibits an obvious enhancement in the tolerance to carbonaceous intermediates and the electocatalytic activity for methanol oxidation reaction (MOR) in comparison to a commercial PtRu/C-JM catalyst and a home-made PtRu/Vulcan catalyst. The MOR mass activity of PtRu/NCNHs (850 mA mg −1 PtRu ) is 2.5 times as high as that of PtRu/C-JM (341 mA mg −1 PtRu ). The MOR specific activity of PtRu/NCNHs is 1.8 times as high as that of PtRu/Vulcan having similar Pt/Ru atomic ratios, specific electrochemical surface areas and particle sizes of PtRu NPs. The electronic interaction between PtRu NPs and NCNHs is responsible for the enhancement in the MOR activity of PtRu/NCNHs

  1. EFFECT OF IMPREGNATION PROCEDURE OF Pt/γ-Al2O3 CATALYSTS UPON CATALYTIC OXIDATION OF CO

    Directory of Open Access Journals (Sweden)

    Triyono Triyono

    2010-06-01

    Full Text Available The oxidation of carbon monoxide by oxygen using two catalysts prepared by two different methods has been investigated. In the first method, catalyst prepared by immersing γ-Al2O3 into the hexa-chloroplatinic acid solution at 80oC for 4 h, resulted Pt/γ-Al2O3 catalyst having platinum highly dispersed on the support. While that of immersing γ-Al2O3 in the hexa-chloroplatinic acid solution at room temperature for 12 h, produced Pt/ γ-Al2O3 catalyst where platinum dispersion was much lower. Catalytic activity test showed that platinum well dispersed on the support enhanced the activity of oxidation of carbon monoxide. The platinum impregnated at room temperature resulted in the poor activity.   Keyword: Catalyst, CO Oxidation, Platinum.

  2. Pt(II) porphyrin modified TiO{sub 2} composites as photocatalysts for efficient 4-NP degradation

    Energy Technology Data Exchange (ETDEWEB)

    Mingyue, Duan [Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xian, Shaanxi 710069 (China); Li Jun, E-mail: junli@nwu.edu.cn [Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xian, Shaanxi 710069 (China); Min, Li [Datang Wujiang Gas Turbine Power Limited Liability Company, Jiangsu 215214 (China); Zengqi, Zhang; Chen, Wang [Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xian, Shaanxi 710069 (China)

    2012-05-01

    Three Pt(II) porphyrins 5,10,15,20-tetra-[2 or 3 or 4-(3-phenoxy)propoxy]phenyl porphyrin]platinum(II) (1-3) were synthesized and characterized spectroscopically. The corresponding Pt(II) porphyrins-TiO{sub 2} composites were then prepared and characterized by means of FT-IR and diffused reflectance spectra, X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The photocatalytic activity of Pt(II) porphyrins-TiO{sub 2} catalyst was investigated by testing the photodegradation of 4-nitrophenol (4-NP) in aqueous solution under irradiation with Xenon lamp. The results indicated that Pt(II) porphyrins greatly enhanced the photocatalytic efficiency of bare TiO{sub 2} in photodegrading the 4-NP, and the distinct space tropisms of peripheral substituents in meso-sites of porphyrin ring led to different results.

  3. Synthesis of Pt-Ru PSB-Py catalysis by {gamma}-irradiation and their electrocatalytic efficiency for methanol oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Yoon, Jung Ah; Sim, Kwang Sik; Choi, Seong Ho [Hannam University, Daejeon (Korea, Republic of); Jung, Sung Hee [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2009-09-15

    We report here that deposition of Pt-Ru catalysis on the surface of core-shell conductive balls by radiation-chemical reduction of Pt and Ru ions, in order to use as catalysis in a fuel cell. The poly(styrene-co-4-vinylphenylboronic acid)-pyrrole (PSB-Py) with core-shell structure was obtained by in situ polymerization of pyrrole in the presence of the poly(styrene-co-4-vinylphenylboronic acid) (PSB). Subsequently, Pt-Ru catalysis were deposited onto PSB-Py ball by {gamma}-irradiation, in the presence/absence of poly(vinypyrolidone) (PVP) to prepare electrocatalysis for a fuel cell. The catalytic efficiency of Pt-Ru PSB-Py catalyst was examined for carbon monoxide (CO) stripping and methanol oxidation.

  4. Synthesis of Pt-Ru PSB-Py catalysis by γ-irradiation and their electrocatalytic efficiency for methanol oxidation

    International Nuclear Information System (INIS)

    Yoon, Jung Ah; Sim, Kwang Sik; Choi, Seong Ho; Jung, Sung Hee

    2009-01-01

    We report here that deposition of Pt-Ru catalysis on the surface of core-shell conductive balls by radiation-chemical reduction of Pt and Ru ions, in order to use as catalysis in a fuel cell. The poly(styrene-co-4-vinylphenylboronic acid)-pyrrole (PSB-Py) with core-shell structure was obtained by in situ polymerization of pyrrole in the presence of the poly(styrene-co-4-vinylphenylboronic acid) (PSB). Subsequently, Pt-Ru catalysis were deposited onto PSB-Py ball by γ-irradiation, in the presence/absence of poly(vinypyrolidone) (PVP) to prepare electrocatalysis for a fuel cell. The catalytic efficiency of Pt-Ru PSB-Py catalyst was examined for carbon monoxide (CO) stripping and methanol oxidation

  5. Catalyst design for clean and efficient fuels

    DEFF Research Database (Denmark)

    Šaric, Manuel

    cobalt promoted MoS2 catalyst. Reactivity of a series of model molecules, found in oil prior to desulfurization, is studied on cobalt promoted MoS2. Such an approach has the potential to explain the underlying processes involved in the removal of sulfur at each specific site of the catalyst. The goal...... is to identify which sites are active towards specific molecules and in getting insight to what the ideal catalyst should look like in terms of morphology. Dimethyl carbonate is an environmentally benign compound that can be used as a solvent and precursor in chemical synthesis or as a fuel and fuel additive...... processes currently used. It is found that noble metals can be used as electrocatalysts for the synthesis of dimethyl carbonate, significantly lowering the potential when using copper instead of gold. Besides being active, copper was found to be selective towards dimethyl carbonate. A non-selective catalyst...

  6. 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...

  7. One-step flame synthesis of an active Pt/TiO2 catalyst for SO2 oxidation

    DEFF Research Database (Denmark)

    Johannessen, Tue; Koutsopoulos, Sotiris

    2002-01-01

    Flame synthesis as a route for production of composite metal oxides has been employed for the one-step synthesis of a supported noble metal catalyst, i.e. a Pt/TiO2 catalyst, by simultaneous combustion of Ti-isopropoxide and platinum acetylacetonate in a quench-cooled flame reactor. The average...... size of the platinum particles supported on aggregated nano-particles of TiO2 is approximately 2 nm. The high SO2-oxidation activity of the catalyst proves that platinum is not hidden in the titania matrix. The flame-produced catalyst showed catalytic activity similar to samples prepared by wet...

  8. 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.

  9. 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.

  10. Efficiency of bimetallic PtPd on polydopamine modified on various carbon supports for alcohol oxidations

    Science.gov (United States)

    Pinithchaisakula, A.; Ounnunkad, K.; Themsirimongkon, S.; Promsawan, N.; Waenkaew, P.; Saipanya, S.

    2017-02-01

    In this work, the preparation, characterization, and electrocatalytic analysis of the catalysts on various carbon substrates for direct alcohol fuel cells were studied. Selected carbons were modified with/without polydopamine (labelled as PDA-C and C) and further metal electrodeposited incorporated onto the glassy carbon (labelled as 5Pt1Pd/PDA-C and 5Pt1Pd/C). Four various carbon materials were used e.g. graphite (G), carbon nanotube (CNT), graphene (GP) and graphene oxide (GO) and the carbons were modified with PDA denoted as PDA-G, PDA-CNT, PDA-GP and PDA-GO, respectively. The transmission electron microscopy (TEM) and scanning electron microscopy (SEM) experimental observation showed narrow size distribution of metal anchored on the PDA-C and C materials. Chemical compositions and oxidation states of the catalysts were determined by X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDX). The catalytic performances for small organic electro-oxidation (e.g. methanol and ethanol) were measured by cyclic voltammetry (CV). Among different PDA-C and C catalysts, monometallic Pt showed less activity than the bimetallic catalysts. Among catalysts with PDA, the 5Pt1Pd/PDA-GO catalyst facilitated methanol and ethanol oxidations with high oxidation currents and If/Ib value and stability with low potentials while among catalysts without PDA, the 5Pt1Pd/CNT provides highest activity and stability. It was found that the catalysts with PDA provided high activity and stability than the catalysts without PDA. The improved catalytic performance of the prepared catalysts could be related to the higher active surface area from polymer modification and bimetallic catalyst system in the catalyst composites.

  11. 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).

  12. 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).

  13. Fabrication and characterization of nanostructured mechanically alloyed Pt-Co catalyst for oxygen gas-diffusion-electrode

    International Nuclear Information System (INIS)

    Pharkya, P.; Farhat, Z.; Czech, E.; Hawthorne, H.; Alfantazi, A.

    2003-01-01

    The use of PEM fuel cells depends largely upon the cost of materials, processing and fabrication. The cost of Pt catalyst is a significant cost of a fuel cell. Alternative low cost catalyst that promotes high rate of oxygen reduction is needed. To achieve this, a mechanochemical technique was employed to refine the catalyst layer structure (i.e. increasing the effective catalyst surface area) and reducing the amount of Pt used, by alloying with a cheaper element. An investigation is carried out to study the relationship between the new catalyst structure refinement, morphology, microstructure and its electrocatalytic behaviour. Nanostructured Pt, Co and Pt 0.2 5 Co 0.75 alloy was fabricated from high purity Pt (99.9%) and Co (99.5%) powders using a Laboratory Planetary Ball Mill 'Pulverisette 6'. Optimum milling conditions, that produce fine, uniform and mechanically alloyed microstructure, were determined during fabrication, by varying process parameters (i.e., rpm, milling time, ball to powder ratio, milling atmosphere, surface-agents and milling/cooling cycle). Mechanically induced chemical and physical reactions and thermal effects were monitored 'in-situ' using a GTM system, which recorded temperature and pressure changes during milling. The alloy catalysts were characterized using TEM, SEM, EDX, XRD and BET techniques. Electrochemical tests were carried out on prepared powders. Exchange currents were determined from a potentiodynamic polarization tests and used to compare relative electrocatalytic behaviour of the new catalyst. Structure/property relationships were discussed and conclusions were drawn on the production of improved low cost catalyst. (author)

  14. 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.

  15. 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

  16. 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.

  17. Ultrasonically treated multi-walled carbon nanotubes (MWCNTs) as PtRu catalyst supports for methanol electrooxidation

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Chunwei; Hu, Xinguo; Wang, Dianlong; Dai, Changsong [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China); Zhang, Liang; Jin, Haibo [School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081 (China); Agathopoulos, Simeon [Department of Materials Science and Engineering, University of Ioannina, GR-451 10 Ioannina (Greece)

    2006-09-29

    In the quest of fabricating supported catalysts, experimental results of transmission electron microscopy, Raman and infrared spectroscopy indicate that ultrasonic treatment effectively functionalizes multi-walled carbon nanotubes (MWCNTs), endowing them with groups that can act as nucleation sites which can favor well-dispersed depositions of PtRu clusters on their surface. Ultrasonic treatment seems to be superior than functionalization via regular refluxing. This is confirmed by the determination of the electrochemistry active surface area (ECA) and the CO-tolerance performance of the PtRu catalysts, measured by adsorbed CO-stripping voltammetry in 0.5M sulfuric acid solution, and the real surface area of the PtRu catalysts, evaluated by Brunauer-Emmett-Teller (BET) measurements. Finally, the effectiveness for methanol oxidation is assessed by cyclic voltammetry (CV) in a sulfuric acid and methanol electrolyte. (author)

  18. Properties of Pt/C catalyst modified by chemical vapor deposition of Cr as a cathode of phosphoric acid fuel cell

    International Nuclear Information System (INIS)

    Seo, Sang Joon; Joh, Han-Ik; Kim, Hyun Tae; Moon, Sang Heup

    2006-01-01

    Cr-modified Pt/C catalysts were prepared by the chemical vapour deposition (CVD) of Cr on Pt/C, and their performance as a cathode of phosphoric acid fuel cell (PAFC) was compared with the case of catalysts containing Cr added by impregnation (IMP). The catalyst prepared by CVD showed a higher activity for oxygen reduction reaction (ORR) than one prepared by IMP. There was an optimum amount of Cr that yielded the maximum mass activity of the catalyst because the gain in the intrinsic activity due to the promotional effect of Cr was counterbalanced by the loss of exposed Pt surface area as a result of the Cr introduction. Nevertheless, the activity increase at the optimum amount of Cr was greater for the CVD catalyst than for the IMP catalyst. Also, the optimum amount of Cr to yield the maximum activity was smaller for the former catalyst [Cr/Pt] CVD = 0.6, than for the latter, [Cr/Pt] IMP = 1.0. The enhancement of the Pt catalyst activity by Cr addition is attributed to two factors: changes in the surface Pt-Pt spacing and the electronic modification of the Pt surface. The formation of a Pt-Cr alloy, as confirmed by X-ray diffraction, decreased the lattice parameter of Pt, which was beneficial to the catalyst activity for ORR. X-ray photoelectron spectroscopy results showed that the binding energies of Pt electrons were shifted to higher energies due to Cr modification. Accordingly, the electron density of Pt was lowered and the Pt-O bond became weak on the Cr-modified catalysts, which was also beneficial to the catalyst activity for ORR. The promotion of oxygen reduction on Cr-modified catalysts was confirmed by measuring the cyclic voltammograms of the catalysts. All the above changes were made more effectively for catalysts prepared by CVD than for those prepared by IMP because the former method allowed Cr to interact more closely with the Pt surface than the latter, which was demonstrated by the characterization of catalysts in this study

  19. Cooperative catalysis designing efficient catalysts for synthesis

    CERN Document Server

    Peters, René

    2015-01-01

    Written by experts in the field, this is a much-needed overview of the rapidly emerging field of cooperative catalysis. The authors focus on the design and development of novel high-performance catalysts for applications in organic synthesis (particularly asymmetric synthesis), covering a broad range of topics, from the latest progress in Lewis acid / Br?nsted base catalysis to e.g. metal-assisted organocatalysis, cooperative metal/enzyme catalysis, and cooperative catalysis in polymerization reactions and on solid surfaces. The chapters are classified according to the type of cooperating acti

  20. Synthesis, characterization and electrochemical studies of Pt- W/C catalyst for polymer electrolyte membrane fuel cells

    International Nuclear Information System (INIS)

    Ahmed, R.; Shahid, S.; Ansari, M. S.

    2013-01-01

    Pt-W/C catalyst was synthesized by slow reduction of platinum and tungsten solutions in the desired ratio with subsequent deposition on the Vulcan carbon already added to the solution. Crystallite size of catalyst was about 9 nm and its density, cell volume, d-spacing and lattice parameter were also calculated. EDX analysis of the catalyst was also done. Electrochemical surface area of the catalyst was determined by cyclic voltammetry (CV). CV of the catalyst was done both in acidic and basic media to find out the peak potential, peak current, specific activity and mass activity of the catalyst. Peak potential versus scan rate plots showed that the electro oxidation of methanol is an irreversible process. Tafel equation was used to plot polarization curves to find out the exchange current density. Higher values of exchange current indicate better catalysts. Specific activities of the catalyst were determined in acidic and basic media and it was found that the specific activity in basic media increased substantially as compared to acidic media. The specific activity in acidic media was 83 mA/mg pt whereas in basic media it was 137mA/mg pt which is a substantial increase. Heterogeneous rate constant in acidic media was 6.15 * 10-6 cm/ s and in basic media it was 4.92 * 10-5 cm/s which is much higher in basic media. In this binary catalyst addition of tungsten has increased the catalytic activity but it is non-noble metal thus will decrease the cost. Stability studies of the catalyst were done upto fifty cycles both in acidic and basic media and was found quite stable in both the media. (author)

  1. Synthesis, characterization and electrochemical studies of Pt-W/C catalyst for polymer electrolyte membrane fuel cells

    International Nuclear Information System (INIS)

    Ahmed, Riaz; Shahid, Saliha; Ansari, Muhammad Shahid

    2014-01-01

    Pt-W/C catalyst was synthesized by slow reduction of platinum and tungsten solutions in the desired ratio with subsequent deposition on the Vulcan carbon already added to the solution. Crystallite size of catalyst was about 9 nm and its density, cell volume, d-spacing and lattice parameter were also calculated. EDX analysis of the catalyst was also done. Electrochemical surface area of the catalyst was determined by cyclic voltammetry (CV). CV of the catalyst was done both in acidic and basic media to find out the peak potential, peak current, specific activity and mass activity of the catalyst. Peak potential versus scan rate plots showed that the electro oxidation of methanol is an irreversible process. Tafel equation was used to plot polarization curves to find out the exchange current density. Higher values of exchange current indicate better catalysts. Specific activities of the catalyst were determined in acidic and basic media and it was found that the specific activity in basic media increased substantially as compared to acidic media. The specific activity in acidic media was 83 mA/mg pt whereas in basic media it was 137mA/mg pt which is a substantial increase. Heterogeneous rate constant in acidic media was 6.15 x 10 −6 cm/ s and in basic media it was 4.92 x 10 −5 cm/s which is much higher in basic media. In this binary catalyst addition of tungsten has increased the catalytic activity but it is non-noble metal thus will decrease the cost. Stability studies of the catalyst were done upto fifty cycles both in acidic and basic media and was found quite stable in both the media

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

    Science.gov (United States)

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

    2015-01-01

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

  3. 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.

  4. Selective catalytic reduction of NOx in lean-burn engine exhaust over a Pt/V/MCM-41 catalyst

    International Nuclear Information System (INIS)

    Jeon, Jong Yeol; Kim, Hee Young; Woo, Seong Ihl

    2003-01-01

    The activities of Pt supported on various metal-substituted MCM-41 (V-, Ti-, Fe-, Al-, Ga-, La-, Co-, Mo-, Ce-, and Zr-MCM-41) and V-impregnated MCM-41 were investigated for the reduction of NO by C 3 H 6 . Among these catalysts, Pt supported on V-impregnated MCM-41 showed the best activity. The maximum conversion of NO into N 2 +N 2 O over this Pt/V/MCM-41 catalyst (Pt=1wt.%, V=3.8wt.%) was 73%, and this maximum conversion was sustained over a temperature range of 70C from 270 to 340C. The high activity of Pt/V/MCM-41 over a broad temperature range resulted from two additional reactions besides the reaction occurring on usual supported Pt, the reaction of NO with surface carbonaceous materials, and the reaction of NO occurring on support V-impregnated MCM-41. The former additional reaction showed an oscillation characteristic, a phenomenon in which the concentrations of parts of reactant and product gases oscillate continuously. At low temperature, some water vapor injected into the reactant gas mixture promoted the reaction occurring on usual supported Pt, whereas at high temperature, it suppressed the additional reaction related to carbonaceous materials. Five-hundred parts per million of SO 2 added to the reactant gas mixture only slightly decreased the NO conversion of Pt/V/MCM-41

  5. Sol-Gel Process for Making Pt-Ru Fuel-Cell Catalysts

    Science.gov (United States)

    Narayanan, Sekharipuram; Valdez, Thomas; Kumta, Prashant; Kim, Y.

    2005-01-01

    A sol-gel process has been developed as a superior alternative to a prior process for making platinum-ruthenium alloy catalysts for electro-oxidation of methanol in fuel cells. The starting materials in the prior process are chloride salts of platinum and ruthenium. The process involves multiple steps, is time-consuming, and yields a Pt-Ru product that has relatively low specific surface area and contains some chloride residue. Low specific surface area translates to incomplete utilization of the catalytic activity that might otherwise be available, while chloride residue further reduces catalytic activity ("poisons" the catalyst). In contrast, the sol-gel process involves fewer steps and less time, does not leave chloride residue, and yields a product of greater specific area and, hence, greater catalytic activity. In this sol-gel process (see figure), the starting materials are platinum(II) acetylacetonate [Pt(C5H7O2)2, also denoted Pt-acac] and ruthenium(III) acetylacetonate [Ru(C5H7O2)3, also denoted Ru-acac]. First, Pt-acac and Ru-acac are dissolved in acetone at the desired concentrations (typically, 0.00338 moles of each salt per 100 mL of acetone) at a temperature of 50 C. A solution of 25 percent tetramethylammonium hydroxide [(CH3)4NOH, also denoted TMAH] in methanol is added to the Pt-acac/Ruacac/ acetone solution to act as a high-molecular-weight hydrolyzing agent. The addition of the TMAH counteracts the undesired tendency of Pt-acac and Ru-acac to precipitate as separate phases during the subsequent evaporation of the solvent, thereby helping to yield a desired homogeneous amorphous gel. The solution is stirred for 10 minutes, then the solvent is evaporated until the solution becomes viscous, eventually transforming into a gel. The viscous gel is dried in air at a temperature of 170 C for about 10 hours. The dried gel is crushed to make a powder that is the immediate precursor of the final catalytic product. The precursor powder is converted to the

  6. Gradient Mn-La-Pt Catalysts with Three-layered Structure for Li-O2 battery

    Science.gov (United States)

    Cai, Kedi; Yang, Rui; Lang, Xiaoshi; Zhang, Qingguo; Wang, Zhenhua; He, Tieshi

    2016-01-01

    Gradient Mn-La-Pt catalysts with three-layered structure of manganese dioxide (MnO2), lanthanum oxide (La2O3), and Platinum (Pt) for Li-O2 battery are prepared in this study. The mass ratio of the catalysts is respectively 5:2:3, 4:2:4, and 3:2:5 (MnO2: La2O3: Pt) which is start from the side of the electrolyte. The relationship between morphology structure and electrochemical performance of gradient catalyst is investigated by energy dispersive spectrometry and constant current charge/discharge test. The Li-O2 battery based on gradient Mn-La-Pt catalysts shows high discharge specific capacity (2707 mAh g−1), specific energy density (8400 Wh kg−1) and long cycle life (56 cycles). The improvement of the Li-O2 battery discharge capacity is attributed to the gradient distribution of MnO2 and Pt and the involvement of La2O3 that can improve the energy density of the battery. More important, this work will also provide new ideas and methods for the research of other metal-air battery. PMID:27731340

  7. Enhancing Pt-Ni/CeO2 performances for ethanol reforming by catalyst supporting on high surface silica

    NARCIS (Netherlands)

    Palma, V.; Ruocco, C; Meloni, E.; Gallucci, F.; Ricca, A.

    2018-01-01

    In this paper, bimetallic Pt-Ni/CeO2 catalysts supported over mesoporous silica were employed for ethanol reforming in the low-temperature range. In particular, catalyst behaviour was investigated under a H2O/C2H5OH/N2 as well as H2O/C2H5OH/AIR mixture between 300 and 600 °C at different space

  8. Characterization of Pt/Sn catalyst for the electrochemical oxidation of methanol

    Energy Technology Data Exchange (ETDEWEB)

    Andrew, M.R.; Drury, J.S.; McNicol, B.D.; Pinnington, C.; Short, R.T.

    1976-03-01

    Pt/Sn electrodeposited catalysts have been prepared, characterized and tested for the electro-oxidation of methanol. Catalyst activities were measured in 3 M H/sub 2/SO/sub 4/ electrolyte between ambient temperature and 95/sup 0/C. Enhancement in specific activity by a factor of about 50 was found over electrodeposited platinum black. This behavior is in contrast to that of alloys of platinum and tin which were found to have very low activities compared with platinum catalysts and to be readily corroded in H/sub 2/SO/sub 4/ electrolyte. ESCA (electron spectroscopy for chemical analysis) studies and Moessbauer spectroscopy showed the majority of the tin in the deposit to be present in an oxidized form. A small amount (approximately 17%) was present as a dilute alloy of tin in platinum. Surface area measurements and X-ray powder diffraction indicated that the increase in activity over platinum black was not attributable to smaller platinum particle size. It seems that the combination of platinum and tin results in a decrease in the poisoning effect by strongly adsorbed organic residues. Whether this arises from the operation of a cyclic Sn(II)/Sn(IV) redox system or from modification of the platinum surface remains unresolved.

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

    Directory of Open Access Journals (Sweden)

    Elena Pastor

    2013-10-01

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

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

    International Nuclear Information System (INIS)

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

    2014-01-01

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

  11. Solvent-free Hydrodeoxygenation of Bio-oil Model Compounds Cyclopentanone and Acetophenone over Flame-made Bimetallic Pt-Pd/ZrO2 Catalysts

    Science.gov (United States)

    Jiang, Yijiao; Büchel, Robert; Huang, Jun; Krumeich, Frank; Pratsinis, Sotiris E.; Baiker, Alfons

    2013-01-01

    Bimetallic Pt-Pd/ZrO2 catalysts with different Pt/Pd atomic ratio and homogeneous dispersion of the metal nanoparticles were prepared in a single step by flame-spray pyrolysis. The catalysts show high activity and tuneable product selectivity for the solvent-free hydrodeoxygenation of the bio-oil model compounds cyclopentanone and acetophenone. PMID:22674738

  12. Improved Oxygen Reduction Activity and Durability of Dealloyed PtCox Catalysts for Proton Exchange Membrane Fuel Cells: Strain, Ligand, and Particle Size Effects

    Science.gov (United States)

    Jia, Qingying; Caldwell, Keegan; Strickland, Kara; Ziegelbauer, Joseph M.; Liu, Zhongyi; Yu, Zhiqiang; Ramaker, David E.; Mukerjee, Sanjeev

    2015-01-01

    The development of active and durable catalysts with reduced platinum content is essential for fuel cell commercialization. Herein we report that the dealloyed PtCo/HSC and PtCo3/HSC nanoparticle (NP) catalysts exhibit the same levels of enhancement in oxygen reduction activity (~4-fold) and durability over pure Pt/C NPs. Surprisingly, ex situ high-angle annular dark field scanning transmission electron microscopy (HAADF STEM) shows that the bulk morphologies of the two catalysts are distinctly different: D-PtCo/HSC catalyst is dominated by NPs with solid Pt shells surrounding a single ordered PtCo core; however, the D-PtCo3/HSC catalyst is dominated by NPs with porous Pt shells surrounding multiple disordered PtCo cores with local concentration of Co. In situ X-ray absorption spectroscopy (XAS) reveals that these two catalysts possess similar Pt–Pt and Pt–Co bond distances and Pt coordination numbers (CNs), despite their dissimilar morphologies. The similar activity of the two catalysts is thus ascribed to their comparable strain, ligand, and particle size effects. Ex situ XAS performed on D-PtCo3/HSC under different voltage cycling stage shows that the continuous dissolution of Co leaves behind the NPs with a Pt-like structure after 30k cycles. The attenuated strain and/or ligand effects caused by Co dissolution are presumably counterbalanced by the particle size effects with particle growth, which likely accounts for the constant specific activity of the catalysts along with voltage cycling. PMID:26413384

  13. Enhanced methanol electro-oxidation activity of Pt/MWCNTs electro-catalyst using manganese oxide deposited on MWCNTs

    International Nuclear Information System (INIS)

    Nouralishahi, Amideddin; Khodadadi, Abbas Ali; Mortazavi, Yadollah; Rashidi, Alimorad; Choolaei, Mohammadmehdi

    2014-01-01

    Highlights: • Promoting effects of manganese oxide (MnO x ) on methanol electro-oxidation over Pt/MWCNTs are studied. • 3.3 times higher activity and improved stability are observed on Pt/MnO x -MWCNTs in MOR. • Both hydrogen spill over and bi-functional mechanism are facilitated in presence of MnO x . • MnO x significantly enhances electrochemical active surface area and dispersion of Pt nanoparticles. • Proton conductivity of electrocatalyst layer is improved upon MnO x incorporation. - Abstract: Electro-oxidation of methanol on platinum nanoparticles supported on a nanocomposite of manganese oxide (MnO x ) and multi-wall carbon nanotubes (MWCNTs) is investigated. The morphology, structure, and chemical composition of the electro-catalysts are characterized by TEM, XRD, EDS, TGA, and H 2 -TPR. The electro-catalytic properties of electrodes are examined by cyclic voltammetry, CO-stripping, electrochemical impedance spectroscopy (EIS), and linear sweep voltammetry (LSV). Compared to Pt/MWCNTs, the Pt/MnO x -MWCNTs electro-catalyst exhibits about 3.3 times higher forward peak current density, during cyclic voltammetry, and 4.6 times higher exchange current density in methanol electro-oxidation reaction. In addition, deposition of manganese oxide onto MWCNTs dramatically increases the electrochemical active surface area from 29.7 for Pt/MWCNTs to 89.4 m 2 g −1 Pt for Pt/MnO x -MWCNTs. The results of long-term cyclic voltammetry show superior stability of Pt nanoparticles upon addition of manganese oxide to the support. Furthermore, the kinetics of formation of the chemisorbed OH groups improves upon manganese oxide incorporation. This leads to a lower onset potential of CO ads oxidation on Pt/MnO x -MWCNTs than on Pt/MWCNTs

  14. Kinetics study of ethanol steam reforming on Pt/CeO{sub 2} based catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Qi, A. [Queen' s-RMC Fuel Cell Research Centre, Kingston, ON (Canada). Dept. of Chemistry and Chemical Engineering; Thurgood, C.; Amphlett, J. [Royal Military College of Canada, Kingston, ON (Canada). Dept. of Chemistry and Chemical Engineering; Peppley, B. [Queens Univ., Kingston, ON (Canada). Dept. of Chemical Engineering

    2009-07-01

    Interest in fuel cell systems operating on fuels derived from renewable energy sources is increasing because they have the potential to produce electricity with high efficiency and minimal emissions of carbon dioxide and other pollutants. Bioethanol is currently produced by the fermentation of non-edible biomass, through conventional means and also through advances in enzyme technology. The authors previously reported on the steam reforming of bioethanol with a stable ceria supported precious metal catalyst, developed in-house. The catalyst had good thermal stability and resisted carbon formation. This paper reported on a more recent kinetic study in which the influence of operating conditions were quantified. The operating conditions included temperature, steam/carbon ratios, and gas hourly velocities. The results of standard catalyst characterization techniques such as BET, TGA, SEM and TPR were also provided. The data was used to drive an empirical rate expression. The study also investigated a potential rate mechanism.

  15. The Performance of the Trickle Bed Reactor Packed with the Pt/SDBC Catalyst Mixture for the CECE Process

    International Nuclear Information System (INIS)

    Seungwoo Paek; Do-Hee Ahn; Heui-Joo Choi; Kwang-Rag Kim; Hongsuk Chung; Sung-Paal Yim; Minsoo Lee; Kyu-Min Song; Soon Hwan Sohn

    2006-01-01

    The CECE (Combined Electrolysis Catalytic Exchange) process with a hydrophobic catalyst is a very effective method to remove small quantities of tritium from light or heavy waste water streams because of its high separation factor and mild operating conditions. The CECE process is composed of an electrolysis cell and a LPCE (Liquid Phase Catalytic Exchange) column. This paper describes the experimental results of the hydrogen isotopic exchange reaction in a trickle bed reactor packed with a hydrophobic catalyst for the development of the LPCE column of the CECE process. The hydrophobic Pt/SDBC (Styrene Divinyl Benzene Copolymer) catalyst has been developed by Korean researchers for the LPCE column of WTRF (Wolsong Tritium Removal Facility). An experimental apparatus was constructed for the various experiments with the different parameters, such as hydrogen flow rate, temperature, and the structure of the mixed catalyst column. The catalyst column was packed with a mixture of hydrophobic catalyst and hydrophilic packing (Dixon gauze ring). The performance of the catalyst bed was expressed as an overall rate constant Kya. To improve the performance of the trickle bed, the modification of the catalyst bed design (changing the shape of the catalyst complex and diluting with inert) has been investigated. (author)

  16. Electrochemical stability and postmortem studies of Pt/SiC catalysts for polymer electrolyte membrane fuel cells

    DEFF Research Database (Denmark)

    Stamatin, Serban Nicolae; Spéder, József; Dhiman, Rajnish

    2015-01-01

    In the presented work, the electrochemical stability of platinized silicon carbide is studied. Postmortem transmission electron microscopy and X-ray photoelectron spectroscopy were used to document the change in the morphology and structure upon potential cycling of Pt/SiC catalysts. Two differen......, silicon carbide undergoes at least mild oxidation if not even silicon leaching....

  17. Influence of alcohol additives in the preparation of electrodeposited Pt-Ru catalysts on oxidized graphite cloths

    International Nuclear Information System (INIS)

    Sieben, Juan Manuel; Duarte, Marta M.E.; Mayer, Carlos E.

    2011-01-01

    Research highlights: → Pt-Ru catalysts were prepared by potential pulse electrodeposition from solutions containing EtOH or EG at pH 2 and 5. → The catalyst particle size, loading and dispersion were influenced by solution pH and alcohol addition. → The deposits prepared at pH 2 exhibited large irregular agglomerates while those prepared at pH 5 presented smaller globular particles. → Pt-Ru system prepared using EG at pH 5 exhibited the best performance for CH 3 OH oxidation. - Abstract: Carbon supported Pt-Ru catalysts were prepared by multiple cycles of potentiostatic pulses from aqueous diluted chloroplatinic acid and ruthenium chloride solutions in the presence of ethanol or ethylene glycol at pH 2 and 5. SEM images showed that the metallic deposit prepared at pH 2 consisted of large irregular agglomerates, whereas smaller globular particles were obtained at pH 5. In addition, the average particle size was considerably decreased in the presence of the stabilizers. The supported Pt-Ru alloys were tested as catalysts for methanol electro-oxidation in acid media. Electrocatalytic activity measurements indicated that the most active electrode was obtained with ethylene glycol as additive at pH 5.

  18. Desorption of Furfural from Bimetallic Pt-Fe Oxides/Alumina Catalysts

    Directory of Open Access Journals (Sweden)

    Gloria Lourdes Dimas-Rivera

    2014-01-01

    Full Text Available In this work, the desorption of furfural, which is a competitive intermediate during the production of biofuel and valuable aromatic compounds, was studied using pure alumina, as well as alumina impregnated with iron and platinum oxides both individually and in combination, using thermogravimetric analysis (TGA. The bimetallic sample exhibited the lowest desorption percentage for furfural. High-resolution transmission electron microscopy (HRTEM imaging revealed the intimate connection between the iron and platinum oxide species on the alumina support. The mechanism of furfural desorption from the Pt-Fe/Al2O3 0.5%-0.5% sample was determined using physisorbed furfural instead of chemisorbed furfural; this mechanism involved the oxidation of the C=O group on furfural by the catalyst. The oxide nanoparticles on γ-Al2O3 support helped to stabilize the furfural molecule on the surface.

  19. Highly efficient and stable catalyst for peroxynitrite decomposition

    Science.gov (United States)

    Yurii V. Geletii; Alan J. Bailey; Jennifer J. Cowan; Ira A. Weinstock; Craig L. Hill

    2001-01-01

    The new cobalt substituted-polyoxometalate K7[CoAlW11O39]•15H2O and the simple CoCl2•6H2O salt are efficient catalysts for peroxynitrite decomposition. These compounds also catalyze the oxidation of ascorbic acid and the nitration of phenol by peroxynitrite.

  20. An efficient, heterogeneous and reusable catalyst for -alkylation of ...

    Indian Academy of Sciences (India)

    Fe(HSO4)3(FHS) was used as an efficient catalyst for the heterogeneous addition of a series of benzylic and allylic alcohols to various -dicarbonyl compounds, which afforded moderate to excellent yields of -alkylated products in 1,2-dichloroethane. In comparison with the previous methods, the present research ...

  1. Role of Pt(0) in bimetallic (Pt,Fe)-FER catalysts in the N2O decomposition

    Czech Academy of Sciences Publication Activity Database

    Tabor, Edyta; Jíša, Kamil; Nováková, Jana; Bastl, Zdeněk; Vondrová, Alena; Závěta, K.; Sobalík, Zdeněk

    2013-01-01

    Roč. 165, JAN 2013 (2013), s. 40-47 ISSN 1387-1811 R&D Projects: GA ČR GA203/09/1627 Institutional support: RVO:61388955 Keywords : bimetallic Pt,Fe- FER * Pt- FER * Pt(0) clusters Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.209, year: 2013

  2. HZSM-5 CATALYST FOR CRACKING PALM OIL TO BIODIESEL: A COMPARATIVE STUDY WITH AND WITHOUT PT AND PD IMPREGNATION

    Directory of Open Access Journals (Sweden)

    Agus Budianto

    2014-05-01

    Full Text Available The Needs of healthy environment and green energy poses a great demand for alternative energy. Biofuel is one of the alternative energy products that are environmentally friendly. Biofuel can be made from plant oils, especially palm oil. Cracking of palm oil into biofuel is constrained by the availability of catalysts. Moreover the available catalyst still gives a low yield. This research aims to study the effect of Pt and Pd impregnation into HZSM-5 catalyst on the catalytic properties. Another aim is to obtain the operating conditions of the catalytic cracking process of palm oil into biofuel which gives the highest yield and selectivity, especially for biodiesel and biogasoline fractions. Catalytic cracking process was carried out in a micro fixed bed reactor with diameter of 1 cm and length of 16 cm. The reactor was filled with a catalyst. The results of the study successfully prove that Pt and Pd impregnated into HZSM-5 catalyst can increase the yield and selectivity of biodiesel. Pd and Pt are highly recommended to increase the yield and selectivity of biodiesel.

  3. Advanced cathode materials for polymer electrolyte fuel cells based on pt/ metal oxides: from model electrodes to catalyst systems.

    Science.gov (United States)

    Fabbri, Emiliana; Pătru, Alexandra; Rabis, Annett; Kötz, Rüdiger; Schmidt, Thomas J

    2014-01-01

    The development of stable catalyst systems for application at the cathode side of polymer electrolyte fuel cells (PEFCs) requires the substitution of the state-of-the-art carbon supports with materials showing high corrosion resistance in a strongly oxidizing environment. Metal oxides in their highest oxidation state can represent viable support materials for the next generation PEFC cathodes. In the present work a multilevel approach has been adopted to investigate the kinetics and the activity of Pt nanoparticles supported on SnO2-based metal oxides. Particularly, model electrodes made of SnO2 thin films supporting Pt nanoparticles, and porous catalyst systems made of Pt nanoparticles supported on Sb-doped SnO2 high surface area powders have been investigated. The present results indicate that SnO2-based supports do not modify the oxygen reduction reaction mechanism on the Pt nanoparticle surface, but rather lead to catalysts with enhanced specific activity compared to Pt/carbon systems. Different reasons for the enhancement in the specific activity are considered and discussed.

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

    Science.gov (United States)

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

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

  5. Poly (p-phenylendiamine/TiO2) nanocomposite promoted Pt/C catalyst for methanol and ethanol electrooxidation in alkaline medium

    International Nuclear Information System (INIS)

    Rostami, Hussein; Rostami, Abbas Ali; Omrani, Abdollah

    2016-01-01

    In the present study, poly (p-phenylendiamine/titanium dioxide) (PpPDA/TiO 2 ) nanocomposites (NCs) were prepared by in situ polymerization of p-phenylenediamine monomer with of different TiO 2 loading. A facile method was developed to promote the electrocatalytic activity of commercial Pt/C catalyst by ultrasonically mixing Pt/C catalyst and PpPDA/TiO 2 NCs. The PpPDA/TiO 2 NC, Pt/C catalyst and composite catalyst of Pt/C + PpPDA/TiO 2 were characterized by scanning electron microscopy (SEM) and Fourier transform infrared (FTIR) spectroscopy. The surface morphology of Pt/C is significantly influenced by the presence of PpPDA/TiO 2 NC as confirmed by SEM observations. Cyclic voltammetry (CV) measurements showed that the PpPDA/TiO 2 NC leads to a significant improvement in the activity and stability of Pt/C for alcohol oxidation especially for ethanol oxidation in alkaline medium. For Pt/C + PpPDA/TiO 2 , the onset potentials shift to negative values by 30 and 160 mV compared to the onset potentials of Pt/C for methanol and ethanol oxidation, respectively. Chronoamperometry (CA) and electrochemical impedance spectroscopy (EIS) results also confirmed that this composite catalyst has superior catalytic performance towards ethanol oxidation compared to the pure Pt/C catalyst.

  6. Preparation and Characterization of Zirconia-Coated Nanodiamonds as a Pt Catalyst Support for Methanol Electro-Oxidation

    Directory of Open Access Journals (Sweden)

    Jing Lu

    2016-12-01

    Full Text Available Zirconia-coated nanodiamond (ZrO2/ND electrode material was successfully prepared by one-step isothermal hydrolyzing from ND-dispersed ZrOCl2·8H2O aqueous solution. High-resolution transmission electron microscopy reveals that a highly conformal and uniform ZrO2 shell was deposited on NDs by this simple method. The coating obtained at 90 °C without further calcination was mainly composed of monoclinic nanocrystalline ZrO2 rather than common amorphous Zr(OH4 clusters. The ZrO2/NDs and pristine ND powder were decorated with platinum (Pt nanoparticles by electrodeposition from 5 mM chloroplatinic acid solution. The electrochemical studies indicate that Pt/ZrO2/ND catalysts have higher electrocatalytic activity and better stability for methanol oxidation than Pt/ND catalysts in acid.

  7. To alloy or not to alloy? Cr modified Pt/C cathode catalysts for PEM fuel cells.

    Science.gov (United States)

    Wells, Peter P; Qian, Yangdong; King, Colin R; Wiltshire, Richard J K; Crabb, Eleanor M; Smart, Lesley E; Thompsett, David; Russell, Andrea E

    2008-01-01

    The cathode electrocatalysts for proton exchange membrane (PEM) fuel cells are commonly platinum and platinum based alloy nanoparticles dispersed on a carbon support. Control over the particle size and composition has, historically, been attained empirically, making systematic studies of the effects of various structural parameters difficult. The controlled surface modification methodology used in this work has enabled the controlled modification of carbon supported Pt nanoparticles by Cr so as to yield nanoalloy particles with defined compositions. Subsequent heat treatment in 5% H2 in N2 resulted in the formation of a distinct Pt3Cr alloy phase which was either restricted to the surface of the particles or present throughout the bulk of the particle structure. Measurement of the oxygen reduction activity of the catalysts was accomplished using the rotating thin film electrode method and the activities obtained were related to the structure of the nanoalloy catalyst particles, largely determined using Cr K edge and Pt L3 edge XAS.

  8. 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

  9. Sn surface-enriched Pt-Sn bimetallic nanoparticles as a selective and stable catalyst for propane dehydrogenation

    KAUST Repository

    Zhu, Haibo

    2014-12-01

    A new one pot, surfactant-free, synthetic route based on the surface organometallic chemistry (SOMC) concept has been developed for the synthesis of Sn surface-enriched Pt-Sn nanoparticles. Bu3SnH selectively reacts with [Pt]-H formed in situ at the surface of Pt nanoparticles, Pt NPs, obtained by reduction of K2PtCl4 by LiB(C2H5)3H. Chemical analysis, 1H MAS and 13C CP/MAS solid-state NMR as well as two-dimensional double-quantum (DQ) and triple-quantum (TQ) experiments show that organo-tin moieties Sn(n-C4H9) are chemically linked to the surface of Pt NPs to produce, in fine, after removal of most of the n-butyl fragment, bimetallic Pt-Sn nanoparticles. The Sn(n-CH2CH2CH2CH3) groups remaining at the surface are believed to stabilize the as-synthesized Pt-Sn NPs, enabling the bimetallic NPs to be well dispersed in THF. Additionally, the Pt-Sn nanoparticles can be supported on MgAl2O4 during the synthesis of the nanoparticles. Some of the Pt-Sn/MgAl2O4 catalyst thus prepared exhibits high activity in PROX of CO and an extremely high selectivity and stability in propane dehydrogenation to propylene. The enhanced activity in propane dehydrogenation is associated with the high concentration of inactive Sn at the surface of Pt nanoparticles which ”isolates” the active Pt atoms. This conclusion is confirmed by XRD, NMR, TEM, and XPS analysis.

  10. Reforming of Ethanol to Produce Hydrogen over PtRuMg/ZrO2 Catalyst

    Directory of Open Access Journals (Sweden)

    Josh Y. Z. Chiou

    2012-01-01

    Full Text Available A modified PtRu/ZrO2 catalyst with Mg is evaluated for the oxidative steam reforming of ethanol (OSRE and the steam reforming of ethanol (SRE. In order to understand the variation in the reaction mechanism on OSRE and SRE, further analysis of both fresh and used catalyst is concentrated on for TEM, TG, Raman, and TPR characterization. The results show that the OSRE reaction requires a higher temperature (∼390°C to achieve 100% ethanol conversion than the SRE reaction (∼2500°C. The distribution of CO is minor for both reactions (< 5% for OSRE, < 1% for SRE. This demonstrates that the water gas shift (WGS reaction is an important side-reaction in the reforming of ethanol to produce H2 and CO2. A comparison of the temperature of WGS (WGS shows it is lower for the SRE reaction (WGS∼250°C for SRE, ~340°C for OSRE.

  11. Electrooxidations of ethanol, acetaldehyde and acetic acid using PtRuSn/C catalysts prepared by modified alcohol-reduction process

    Energy Technology Data Exchange (ETDEWEB)

    Wu, Gang [Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208 (United States); Swaidan, Raja [Department of Chemical Engineering, Cooper Union, New York, NY 10003 (United States); Cui, Guofeng [School of Chemistry and Chemical Engineering, Sun-Yat Sen University, Guangzhou 510275 (China)

    2007-10-11

    Well-dispersed ternary PtRuSn catalysts of various atomic ratios (60:30:10, 60:20:20 and 60:10:30) were deposited onto carbon using modified alcohol-reduction process for electrochemical oxidation of ethanol. The alloy phase structure and surface morphology for each variation of the PtRuSn/C catalysts were determined by XRD and HRTEM. In order to evaluate the contributions of Ru and Sn in the different stages of ethanol oxidation, electrochemical oxidations of adsorbed CO, ethanol, acetaldehyde and acetic acid were performed on each PtRuSn/C catalyst. The results indicated that the Ru-rich PtRuSn/C catalyst (60:30:10) exhibited the lowest onset potential for the electrooxidations of adsorbed CO, ethanol and acetaldehyde, revealing that the removal through oxidation of the intermediate C{sub 1} and C{sub 2} species from Pt sites is primarily attributed to the Ru and Pt{sub 3}Sn alloy structures. However, for the overall oxidation of ethanol, the Sn-rich PtRuSn/C catalyst (60:10:30) containing PtSn phase and SnO{sub 2} structure is favorable for the activation of C-C bond breaking, thereby generating higher current density (mass activity) at higher potentials. Moreover, in the electrooxidation of acetic acid, a remarkable improvement for oxidizing acetic acid to C{sub 1} species was observed in the Sn-rich PtRuSn/C catalyst (60:10:30), while the Ru-rich PtRuSn/C catalyst (60:30:10) was almost incapable of breaking the C-C bond to further oxidize acetic acid. The possible reasons for the different reactivities on the studied PtRuSn/C catalysts were discussed based on the removal of intermediates and activation of the C-C bonds on the different surfaces. (author)

  12. Kinetics and mechanistic study of n-alkane hydroisomerization reaction on Pt-doped γ-alumina catalyst

    Directory of Open Access Journals (Sweden)

    Abhishek Dhar

    2017-12-01

    Full Text Available The catalysts γ-alumina (GA, the reference catalyst and Pt doped γ-alumina (PGA-s were synthesized using a simple sol-gel technique, in which at first preparation of porous base (GA, then impregnation of platinum salt over the base and finally reduction of platinum in the surface of the support were done. These catalysts prepared in different mole ratios of Pt:Al as 2:1, 1:1 and 1:2 are named as PGA-1, PGA-2 and PGA-3 respectively. The isomerization of n-alkanes (n-hexane, n-heptane and n-octane were investigated over the synthesized catalysts. The 2-methyl pentane (2-MP, 2,2-dimethyl pentane (2,2-DMP and 2,3-dimethyl hexane (2,3-DMH are the major products of respective isomerization of n-hexane, n-heptane and n-octane, besides a small amount of other branched isomers are also produced. The product distribution is comparable to that reported for Pt based other catalysts. The optimal mole ratios of Pt:Al is 1:1 (PGA-2 gives quite good catalytic activity for isomerization of n-alkane. Even through in reusability study, PGA-2 gives better performance than others. We have mainly focused on kinetic study, reaction mechanism behind isomerization and calculated the order of reactions and activation energies of the isomerization reactions in the present work. Keywords: Isomerization, n-alkanes, Catalyst, Reaction mechanism, Kinetics study, Activation energy

  13. 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.

  14. Enhanced methanol electro-oxidation reaction on Pt-CoO{sub x}/MWCNTs hybrid electro-catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Nouralishahi, Amideddin, E-mail: Nouralishahi@ut.ac.ir [Catalysis and Nanostructured Materials Research Laboratory, School of Chemical Engineering, University of Tehran, P.O. Box 11155/4563, Tehran (Iran, Islamic Republic of); Caspian Faculty of Engineering, University of Tehran, P.O. Box 43841-119, Rezvanshahr (Iran, Islamic Republic of); Catalysis and Nanotechnology Research Division, Research Institute of Petroleum Industry (RIPI), P.O. Box 14665-1998, Tehran (Iran, Islamic Republic of); Rashidi, Ali Morad, E-mail: Rashidiam@ripi.ir [Catalysis and Nanotechnology Research Division, Research Institute of Petroleum Industry (RIPI), P.O. Box 14665-1998, Tehran (Iran, Islamic Republic of); Mortazavi, Yadollah, E-mail: Mortazav@ut.ac.ir [Catalysis and Nanostructured Materials Research Laboratory, School of Chemical Engineering, University of Tehran, P.O. Box 11155/4563, Tehran (Iran, Islamic Republic of); Khodadadi, Abbas Ali, E-mail: Khodadad@ut.ac.ir [Catalysis and Nanostructured Materials Research Laboratory, School of Chemical Engineering, University of Tehran, P.O. Box 11155/4563, Tehran (Iran, Islamic Republic of); Choolaei, Mohammadmehdi, E-mail: Choolaeimm@ripi.ir [Catalysis and Nanotechnology Research Division, Research Institute of Petroleum Industry (RIPI), P.O. Box 14665-1998, Tehran (Iran, Islamic Republic of)

    2015-04-30

    Highlights: • Promoting effects of Cobalt oxide on methanol electro-oxidation over Pt/MWCNTs are investigated. • Higher activity, about 2.9 times, and enhanced stability are observed on Pt-CoO{sub x}/MWCNTs. • Electrochemical active surface area of Pt nanoparticles is significantly improved upon CoO{sub x} addition. • Bi-functional mechanism is facilitated in presence of CoO{sub x}. - Abstract: The electro-catalytic behavior of Pt-CoO{sub x}/MWCNTs in methanol electro-oxidation reaction (MOR) is investigated and compared to that of Pt/MWCNTs. The electro-catalysts were synthesized by an impregnation method using NaBH{sub 4} as the reducing agent. The morphological and physical characteristics of samples are examined by XRD, TEM, ICP and EDS techniques. In the presence of CoO{sub x}, Pt nanoparticles were highly distributed on the support with an average particle size of 2 nm, an obvious decrease from 5.1 nm for Pt/MWCNTs. Cyclic voltammetry, CO-stripping, Chronoamperometry, and electrochemical impedance spectroscopy (EIS) measurements are used to study the electrochemical behavior of the electro-catalysts. The results revealed a considerable enhancement in the oxidation kinetics of CO{sub ads} on Pt active sites by the participation of CoO{sub x}. Compared to Pt/MWCNTs, Pt-CoO{sub x}/MWCNTs sample has a larger electrochemical active surface area (ECSA) and higher electro-catalytic activity and stability toward methanol electro-oxidation. According to the results of cyclic voltammetry, the forward anodic peak current density enhances more than 89% at the optimum atomic ratio of Pt:Co = 2:1. Furthermore, inclusion of cobalt oxide species causes the onset potential of methanol electro-oxidation reaction to shift 84 mV to negative values compared to that on Pt/MWCNTs. Based on EIS data, dehydrogenation of methanol is the rate-determining step of MOR on both Pt/MWCNTs and Pt-CoO{sub x}/MWCNTs, at small overpotentials. However, at higher overpotentials, the

  15. Characterization of Industrial Pt-Sn/Al2O3 Catalyst and Transient Product Formations during Propane Dehydrogenation

    Directory of Open Access Journals (Sweden)

    Kah Sing Ho

    2013-06-01

    Full Text Available The major problem plaguing propane dehydrogenation process is the coke formation on the Pt-Sn/Al2O3 catalyst which leads to catalyst deactivation. Due to information paucity, the physicochemical characteristics of the commercially obtained regenerated Pt-Sn/Al2O3 catalyst (operated in moving bed reactor and coke formation at different temperatures of reaction were discussed. The physicochemical characterization of regenerated catalyst gave a BET surface area of 104.0 m2/g with graphitic carbon content of 8.0% indicative of incomplete carbon gasification during the industrial propylene production. Effect of temperatures on coke formation was identified by studying the product yield via temperature-programmed reaction carried out at 500oC, 600oC and 700oC. It was found that ethylene was precursor to carbon laydown while propylene tends to crack into methane. Post reaction, the spent catalyst possessed relatively lower surface area and pore radius whilst exhibited higher carbon content (31.80% at 700oC compared to the regenerated catalyst. Significantly, current studies also found that higher reaction temperatures favoured the coke formation. Consequently, the propylene yield has decreased with reaction temperature. © 2013 BCREC UNDIP. All rights reservedReceived: 10th March 2013; Revised: 28th April 2013; Accepted: 6th May 2013[How to Cite: Kah, S.H., Joanna Jo, E.C., Sim, Y.C., Chin, K.C. (2013. Characterization of Industrial Pt-Sn/Al2O3 Catalyst and Transient Product Formations during Propane Dehydrogenation. Bulletin of Chemical Reaction Engineering & Catalysis, 8 (1: 77-82. (doi:10.9767/bcrec.8.1.4569.77-82][Permalink/DOI: http://dx.doi.org/10.9767/bcrec.8.1.4569.77-82] | View in  |

  16. On the activation of Pt/Al2O3 catalysts in HC-SCR by sintering. Determination of redox-active sites using Multitrack

    International Nuclear Information System (INIS)

    Vaccaro, A.R.; Mul, G.; Moulijn, J.A.; Perez-Ramirez, J.

    2003-01-01

    A highly dispersed Pt/Al 2 O 3 catalyst was used for the selective catalytic reduction of NO x using propene (HC-SCR). Contact with the reaction gas mixture led to a significant activation of the catalyst at temperatures above 523K. According to CO chemisorption data and HRTEM analysis, Pt particles on the activated catalyst had sintered. The redox behavior of the fresh and sintered catalysts was investigated using Multitrack, a TAP-like pulse reactor. If Pt particles on the catalyst are highly dispersed (average size below =2nm), only a small part (=10%) of the total number of Pt surface sites as determined by CO chemisorption (Pt surf ) participates in H 2 /O 2 redox cycles (Pt surf,redox ) in Multitrack conditions. For a sintered catalyst, with an average particle size of 2.7nm, the number of Pt surf and Pt surf,redox sites are in good agreement. Similar results were obtained for both catalysts using NO as the oxidant. The low number of Pt surf,redox sites on highly dispersed Pt/Al 2 O 3 is explained by the presence of a kinetically more stable-probably ionic-form of Pt-O bonds on all surface sites of the smaller Pt particles, including corner, edge and terrace sites. When the average particle size shifts to =2.7nm, the kinetic stability of all Pt-O bonds is collectively decreased, enabling the participation of all Pt surface sites in the redox cycles. A linear correlation between the NO x conversion in HC-SCR, and the amount of Pt surf,redox was found. This suggests that redox-active Pt sites are necessary for catalytic activity. In addition, the correlation could be significantly improved by assuming that Pt surf,terrace sites of the particles larger than 2.7nm are mainly responsible for HC-SCR activity in steady state conditions. Implications of these results for the pathway of HC-SCR over Pt catalysts are discussed

  17. Gram-Scale Synthesis of Highly Active and Durable Octahedral PtNi Nanoparticle Catalysts for Proton Exchange Membrane Fuel Cell

    DEFF Research Database (Denmark)

    Choi, Juhyuk; Jang, Jue-Hyuk; Roh, Chi-Woo

    2018-01-01

    for the commercialization of PEMFCs. In this study, we focus on gram-scale synthesis of octahedral PtNi nanoparticles with Pt overlayers (PtNi@Pt) supported on the carbon, resulting in enhanced catalytic activity and durability. Such PtNi@Pt catalysts show high mass activity (1.24 A mgPt−1) at 0.9 V (vs RHE) for the ORR......Proton exchange membrane fuel cells (PEMFC) are regarded as a promising renewable energy source for a future hydrogen energy society. However, highly active and durable catalysts are required for the PEMFCs because of their intrinsic high overpotential at the cathode and operation under the acidic...... condition for oxygen reduction reaction (ORR). Since the discovery of the exceptionally high surface activity of Pt3Ni(111), the octahedral PtNi nanoparticles have been synthesized and tested. Nonetheless, their milligram-scale synthesis method and poor durability make them unsuitable...

  18. Uniform Pt Nanoparticles Incorporated into Reduced Graphene Oxides with MoO_3 as Advanced Anode Catalysts for Methanol Electro-oxidation

    International Nuclear Information System (INIS)

    Hao, Yanfei; Wang, Xudan; Zheng, Yuanyuan; Shen, Jianfeng; Yuan, Junhua; Wang, Ai-jun; Niu, Li; Huang, Shengtang

    2016-01-01

    Highlights: • Pt nanoparticles were uniformly deposited on graphene with MoO_3. Their size can be tuned by controlling MoO_3 loading. These Pt catalysts are high active on methanol oxidation. They also show high tolerance to CO poisoning. - Abstract: Pt nanoparticles (NPs) were uniformly deposited on the reduced graphene oxides (RGOs) by one-pot thermoreduction strategy with assist of MoO_3. MoO_3 can significantly reduce the size of Pt NPs on RGOs. These Pt NPs can be averaged to be 3.0 to 4.1 nm with MoO_3 loading from 27.4 to 8.8%. Without MoO_3, the size of Pt NPs can reach up to 15.2 nm. In addition, MoO_3 in Pt-MoO_3/RGO catalysts conducts a surface-confined reversible electron transfer. And the Pt-MoO_3/RGO catalysts show strong resistance to CO poisoning and high activity towards methanol oxidation reaction (MOR). Among these Pt-based catalysts, Pt-MoO_3/RGO catalysts with 16.5% MoO_3 loading possess a largest MOR current up to 610 mA mg"−"1 Pt with a smallest deteriorate rate of 0.000425 s"−"1 polarizing for 5000 s at 0.65 V. These results demonstrate commercial feasibility for Pt catalysts to reduce significantly the amount of precious metals Pt in parallel to maintain a high MOR activity and CO tolerance.

  19. Macrodynamic study and catalytic reduction of NO by ammonia under mild conditions over Pt-La-Ce-O/Al2O3 catalysts

    International Nuclear Information System (INIS)

    Wang, Yanhui; Zhu, Jingli; Ma, Runyu

    2007-01-01

    Catalytic reduction of NO using ammonia upon series prepared catalysts under 423-573 K in a fixed bed reactor was investigated. Results showed that the performance of supported platinum catalyst could be improved by addition of La and Ce to it. Experimental studies indicated that the suitable molar ratio of Pt:La:Ce would be 1.0:3.78:3.56, Pt-La-Ce (c). Results also found Pt-La-Ce (c) catalyst had good stability and tolerance to certain amounts of sulfur compounds under the used experimental conditions. Characterization for the fresh and used catalysts showed the Pt-La-Ce (c) catalyst had a stable structure. In addition, based on experimental data and using a nonlinear regression algorithm method, an empirical macrodynamic equation was obtained in this study

  20. 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.)

  1. Facile preparation of a Pt/Prussian blue/graphene composite and its application as an enhanced catalyst for methanol oxidation

    International Nuclear Information System (INIS)

    Wang, Zonghua; Shi, Guoyu; Xia, Jianfei; Xia, Yanzhi; Zhang, Feifei; Xia, Lin; Song, Daimin; Liu, Jingquan; Li, Yanhui; Xia, Linhua; Brito, Manuel E.

    2014-01-01

    Graphical abstract: - Highlights: • Pt/Prussian blue/graphene catalyst was easily synthesized by the sequential electrodeposition method. • Prussian blue can promote the homogeneous growth of small Pt nanoparticles. • The as-made catalyst exhibited enhanced electro-catalytic performance for methanol oxidation. • The interplay of Prussian blue and Pt plays a significant role in reducing CO poisoning of the catalyst. - Abstract: Graphene nanosheets (GN) are modified by electrodeposition of Prussian blue (PB) followed by shape-regulated depositing of small Pt nanoparticles via the interaction between PB and PtCl 6 2− to form a novel catalyst Pt/PB/GN. The Pt/PB/GN composite exhibits significantly enhanced electrocatalytic activity with a mass activity of 445 mA mg −1 Pt (at 0.68 V vs. SCE) and high stability towards methanol oxidation. The high catalytic activity can be attributed to the unique porous architecture and peculiar electrical property of Prussian blue integrated with graphene layers which can not only well accommodate Pt nanoparticles but also provide multidimensional pathways to facilitate the mass and electron transport for methanol oxidation. This strategy can be readily extended to fabrication of other graphene-based hybrid supports for precious metal catalysts in fuel cell applications

  2. Characterization of Pt catalysts supported in mixed oxides; Caracterizacion de catalizadores de Pt soportado en oxidos mixtos

    Energy Technology Data Exchange (ETDEWEB)

    Perez H, R.; Garcia C, M.A.; Gomez C, A.; Diaz, G. [Instituto Nacional de Investigaciones Nucleares, A.P. 18-1027, 11801 Mexico D.F. (Mexico)

    2000-07-01

    The catalytic supports TiO{sub 2}, ZrO{sub 2} and TiO{sub 2}-ZrO{sub 2} were prepared by the sol-gel technique. The incorporation of Pt to the supports was by the classical impregnation method. The catalytic materials were characterized (Pt/TiO{sub 2}, Pt/ZrO{sub 2} and Pt/TiO{sub 2}-ZrO{sub 2}) by diverse techniques to determine: the texture (BET), evolution of the catalytic materials synthesised after drying and calcination (Infrared spectroscopy) and by Thermogravimetric analysis. (Author)

  3. Structural and electrochemical characterization of carbon supported Pt-Pr catalysts for direct ethanol fuel cells prepared using a modified formic acid method in a CO atmosphere.

    Science.gov (United States)

    Corradini, Patricia Gon; Antolini, Ermete; Perez, Joelma

    2013-07-28

    Pt-Pr/C electrocatalysts were prepared using a modified formic acid method, and their activity for carbon monoxide and ethanol oxidation was compared to Pt/C. No appreciable alloy formation was detected by XRD analysis. By TEM measurements it was found that Pt particle size increases with an increasing Pr content in the catalysts and with decreasing metal precursor addition time. XPS measurements indicated Pt segregation on the catalyst surface and the presence of Pr2O3 and PrO2 oxides. The addition of Pr increased the electro-catalytic activity of Pt for both CO and CH3CH2OH oxidation. The enhanced activity of Pt-Pr/C catalysts was ascribed to both an electronic effect, caused by the presence of Pr2O3, and the bi-functional mechanism, caused by the presence of PrO2.

  4. Preparation Effects on the Performance of Silica-Doped Hydrous Titanium Oxide (HTO:Si)-Supported Pt Catalysts for Lean-Burn NOx Reduction by Hydrocarbons; TOPICAL

    International Nuclear Information System (INIS)

    GARDNER, TIMOTHY J.; MCLAUGHLIN, LINDA I.; MOWERY, DEBORAH L.; SANDOVAL, RONALD S.

    2002-01-01

    This report describes the development of bulk hydrous titanium oxide (HTO)- and silica-doped hydrous titanium oxide (HTO:Si)-supported Pt catalysts for lean-burn NOx catalyst applications. The effects of various preparation methods, including both anion and cation exchange, and specifically the effect of Na content on the performance of Pt/HTO:Si catalysts, were evaluated. Pt/HTO:Si catalysts with low Na content ( and lt; 0.5 wt.%) were found to be very active for NOx reduction in simulated lean-burn exhaust environments utilizing propylene as the major reductant species. The activity and performance of these low Na Pt/HTO:Si catalysts were comparable to supported Pt catalysts prepared using conventional oxide or zeolite supports. In ramp down temperature profile test conditions, Pt/HTO:Si catalysts with Na contents in the range of 3-5 wt.% showed a wide temperature window of appreciable NOx conversion relative to low Na Pt/HTO:Si catalysts. Full reactant species analysis using both ramp up and isothermal test conditions with the high Na Pt/HTO:Si catalysts, as well as diffuse reflectance FTIR studies, showed that this phenomenon was related to transient NOx storage effects associated with NaNO(sub 2)/NaNO(sub 3) formation. These nitrite/nitrate species were found to decompose and release NOx at temperatures above 300 C in the reaction environment (ramp up profile). A separate NOx uptake experiment at 275 C in NO/N(sub 2)/O(sub 2) showed that the Na phase was inefficiently utilized for NOx storage. Steady state tests showed that the effect of increased Na content was to delay NOx light-off and to decrease the maximum NOx conversion. Similar results were observed for high K Pt/HTO:Si catalysts, and the effects of high alkali content were found to be independent of the sample preparation technique. Catalyst characterization (BET surface area, H(sub 2) chemisorption, and transmission electron microscopy) was performed to elucidate differences between the HTO- and HTO

  5. Novel Pt-Ru nanoparticles formed by vapour deposition as efficient electrocatalyst for methanol oxidation

    International Nuclear Information System (INIS)

    Sivakumar, Pasupathi; Tricoli, Vincenzo

    2006-01-01

    The methods developed and described in paper-part I are employed to prepare nanometer size Pt-Ru particles on a Vulcan[reg] XC72R substrate with controlled metal loading. Transmission Electron Microscopy (TEM) confirmed uniform particles size (average diameter 2 nm) and homogeneous dispersion of the particles over the substrate. Energy Dispersive X-ray absorption (EDX) analysis confirmed the compositional homogeneity. The catalytic activity of these supported nanoparticles with regard to methanol electrooxidation is investigated using cyclic voltammetry (CV), chronoamperometry (CA) and CO-stripping voltammetry techniques at temperatures between 25 and 60 deg. C. Such investigation concerns supported catalysts prepared with ca. 10 and 18 wt.% overall metal loading (Pt + Ru) onto the Vulca[reg] XC72R substrate. Comparative testing of our catalysts and a commercial Pt-Ru/Vulcan reveals markedly superior activity for our catalysts. In fact, we observe for the latter a five-fold increase of the oxidation current as compared to a commercial Pt-Ru/Vulcan with equal metal loading. One of the reasons for the greater activity is found to be the very high dispersion of the metals over the substrate, i.e. the large surface area of the active phase. Other reasons are plausibly ascribable to the varied Pt/Ru composition and/or reduced presence of contaminants at the catalyst surface

  6. Hydroisomerization of n-Pentane over Pt/Mordenite Catalyst: Effect of Feed Composition and Process Conditions

    Directory of Open Access Journals (Sweden)

    Behrouz Bayati

    2016-04-01

    Full Text Available The hydroisomerization of pure n-pentane over H-mordenite supported Pt-catalyst was investigated in a fixed bed reactor by changing reaction parameters such as temperature, pressure, and WHSV, as well as the H2/HC ratio. The maximum yield of isopentane over Pt/mordenite catalyst was achieved at 220 °C and a relatively low reaction pressure. To address the effect of feed composition on the catalytic performance of the samples, the catalysts were assessed for activity and selectivity in the isomerization of a mixture consisting of n-pentane (70 wt.% and isopentane (30 wt.% at 220 °C. The effects of pressure, WHSV, and H2/HC ratio on the catalyst performance were also studied using binary mixtures of the pentane isomers as a feedstock. It was observed that an effect of WHSV and H2/HC on the catalytic performance was similar to its behavior in pure n-pentane isomerization, while the conversion of n-pentane in the binary mixture showed a different trend and had a minimum value at 1.5 bar. It could be due to the presence of isopentane in feed and adsorption phenomenon of binary mixture on mordenite-supported catalyst.

  7. 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.

  8. 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.

  9. The performance of a trickle-bed reactor packed with a Pt/SDBC catalyst mixture for the CECE process

    International Nuclear Information System (INIS)

    Paek, Seungwoo; Ahn, Do-Hee; Choi, Heui-Joo; Kim, Kwang-Rag; Lee, Minsoo; Yim, Sung-Paal; Chung, Hongsuk; Song, Kyu-Min; Sohn, Soon Hwan

    2007-01-01

    The combined electrolysis and catalytic exchange (CECE) process with a hydrophobic catalyst is a very effective method to remove small quantities of tritium from light or heavy wastewater streams because of its high separation factor and mild operating conditions. A hydrophobic platinum/styrene-divinyl benzene copolymer (Pt/SDBC) catalyst which was developed for the liquid-phase catalytic exchange (LPCE) column of the Wolsong tritium removal facility (WTRF) has been tested in a trickle bed reactor for the design of the CECE process. An experimental apparatus has been built for the testing of the catalyst at various temperatures and gas velocities. The catalyst column was packed with a mixture of a hydrophobic catalyst and a hydrophilic packing (Dixon gauze ring) to improve the liquid distribution and vapor/liquid transfer area. Many tests have been carried out at Korea Atomic Energy Research Institute (KAERI) to measure the activity of the catalyst, K y a (1 s -1 ), under various operating conditions. K y a increases with the hydrogen flow rates in the range of 0.4-1.6 m s -1 at STP. The height of the catalyst column was determined from these K y a values according to the reaction temperatures and hydrogen flow rates

  10. The performance of a trickle-bed reactor packed with a Pt/SDBC catalyst mixture for the CECE process

    Energy Technology Data Exchange (ETDEWEB)

    Paek, Seungwoo [Korea Atomic Energy Research Institute, 150 Deokjin-dong, Yuseong-gu, Daejeon 305-353 (Korea, Republic of)], E-mail: swpaek@kaeri.re.kr; Ahn, Do-Hee; Choi, Heui-Joo; Kim, Kwang-Rag; Lee, Minsoo; Yim, Sung-Paal; Chung, Hongsuk [Korea Atomic Energy Research Institute, 150 Deokjin-dong, Yuseong-gu, Daejeon 305-353 (Korea, Republic of); Song, Kyu-Min; Sohn, Soon Hwan [Korea Electric Power Research Institute, 103-16 Munji-dong, Yuseong-gu, Daejeon 305-380 (Korea, Republic of)

    2007-10-15

    The combined electrolysis and catalytic exchange (CECE) process with a hydrophobic catalyst is a very effective method to remove small quantities of tritium from light or heavy wastewater streams because of its high separation factor and mild operating conditions. A hydrophobic platinum/styrene-divinyl benzene copolymer (Pt/SDBC) catalyst which was developed for the liquid-phase catalytic exchange (LPCE) column of the Wolsong tritium removal facility (WTRF) has been tested in a trickle bed reactor for the design of the CECE process. An experimental apparatus has been built for the testing of the catalyst at various temperatures and gas velocities. The catalyst column was packed with a mixture of a hydrophobic catalyst and a hydrophilic packing (Dixon gauze ring) to improve the liquid distribution and vapor/liquid transfer area. Many tests have been carried out at Korea Atomic Energy Research Institute (KAERI) to measure the activity of the catalyst, K{sub y}a (1 s{sup -1}), under various operating conditions. K{sub y}a increases with the hydrogen flow rates in the range of 0.4-1.6 m s{sup -1} at STP. The height of the catalyst column was determined from these K{sub y}a values according to the reaction temperatures and hydrogen flow rates.

  11. Pt hierarchical structure catalysts on BaTiO{sub 3}/Ti electrode for methanol and ethanol electrooxidations

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Chenguo; He, Xiaoshan; Xia, Chuanhui [Department of Applied Physics, Chongqing University, Chongqing 400044 (China)

    2010-03-15

    Electrooxidations of methanol and ethanol have been investigated on different Pt catalytic titanium-supported electrodes in both acidic and alkaline media using cyclic voltammetry. BaTiO{sub 3} is used for the first time to make a nanoscaled roughness on the surface of Ti foil in order to effectively deposit Pt hierarchical structure and block foulness in solution reactions. The morphology of BaTiO{sub 3} nanocube on Ti foil, Pt catalysts deposited on BaTiO{sub 3}/Ti and Ti foil electrodes are characterized by field emission scanning electron microscopy. The results indicate that Pt nanoflowers can be effectively grown on the Ti foil covered with 1 {mu}m layer of BaTiO{sub 3} nanocubes and the catalytic oxidation behaviors to methanol and ethanol are much better than those of the Pt/Ti electrode as Pt nanoparticles can hardly be deposited on the smooth surface of the Ti foil. The Pt/BaTiO{sub 3}/Ti electrode could be adopted as excellent catalytic anode in fuel cells. (author)

  12. Atomic Layer Deposition of Pt Nanoparticles within the Cages of MIL-101: A Mild and Recyclable Hydrogenation Catalyst

    Directory of Open Access Journals (Sweden)

    Karen Leus

    2016-03-01

    Full Text Available We present the in situ synthesis of Pt nanoparticles within MIL-101-Cr (MIL = Materials Institute Lavoisier by means of atomic layer deposition (ALD. The obtained Pt@MIL-101 materials were characterized by means of N2 adsorption and X-ray powder diffraction (XRPD measurements, showing that the structure of the metal organic framework was well preserved during the ALD deposition. X-ray fluorescence (XRF and transmission electron microscopy (TEM analysis confirmed the deposition of highly dispersed Pt nanoparticles with sizes determined by the MIL-101-Cr pore sizes and with an increased Pt loading for an increasing number of ALD cycles. The Pt@MIL-101 material was examined as catalyst in the hydrogenation of different linear and cyclic olefins at room temperature, showing full conversion for each substrate. Moreover, even under solvent free conditions, full conversion of the substrate was observed. A high concentration test has been performed showing that the Pt@MIL-101 is stable for a long reaction time without loss of activity, crystallinity and with very low Pt leaching.

  13. Growth of vertically aligned single-walled carbon nanotubes with metallic chirality through faceted FePt-Au catalysts

    Science.gov (United States)

    Ohashi, Toshiyuki; Iwama, Hiroki; Shima, Toshiyuki

    2016-02-01

    Direct synthesis of vertically aligned metallic single-walled carbon nanotubes (m-SWCNT forests) is a difficult challenge. We have successfully synthesized m-SWCNT forests using faceted iron platinum-gold catalysts epitaxially grown on a single crystalline magnesium oxide substrate. The metallic content of the forests estimated by Raman spectroscopy reaches 90%. From the standpoint of growth rate of the forests, the growth mechanism is probably based on the catalyst of solid state. It is suggested that preferential growth of m-SWCNTs is achieved when both factors are satisfied, namely, {111} dominant octahedral facet and ideal size (fine particles) of FePt particles.

  14. In situ Ru K-edge EXAFS of CO adsorption on a Ru modified Pt/C fuel cell catalyst

    International Nuclear Information System (INIS)

    Rose, Abigail; Bilsborrow, Robert; King, Colin R.; Ravikumar, M.K.; Qian Yangdong; Wiltshire, Richard J.K.; Crabb, Eleanor M.; Russell, Andrea E.

    2009-01-01

    The Ru-CO bond of CO adsorbed on a Ru modified Pt/C fuel cell catalyst has been directly probed by in situ EXAFS at the Ru K-edge, providing evidence of a CO:metal surface atom ratio greater than 1:1 and that CO is adsorbed at bridging sites associated with Ru atoms at the surface of the catalyst nanoparticles. This result illustrates the limitations of single crystal models as representations of the bonding of adsorbed species at nanoparticle surfaces.

  15. Controlling fuel crossover and hydration in ultrathin proton exchange membrane-based fuel cells using Pt-nanosheet catalysts

    DEFF Research Database (Denmark)

    Wang, Rujie; Zhang, Wenjing (Angela); He, Gaohong

    2014-01-01

    and provided in situ hydration inside Nafion membranes to maintain their proton conductivity level. Furthermore, LDH nanosheets reinforced the Nafion membranes, with 181% improvement in tensile modulus and 166% improvement in yield strength. In a hydrogen fuel cell running with dry fuel, the membrane......An ultra-thin proton exchange membrane with Pt-nanosheet catalysts was designed for a self-humidifying fuel cell running on H2 and O2. In this design, an ultra-thin Nafion membrane was used to reduce ohmic resistance. Pt nanocatalysts were uniformly anchored on exfoliated, layered double hydroxide...

  16. Hydrogen from bioethanol on Pt/Hydrotalcite catalysts stabilized with WOx; Hidrogeno a partir de bioetanol sobre catalizadores de Pt/hidrotalcita estabilizados con WOx

    Energy Technology Data Exchange (ETDEWEB)

    Ortiz, M.A.; Contreras, J.L. [Universidad Autonoma Metropolitana-Azcapotzalco, Mexico, D.F. (Mexico)]. E-mail: jlcl@correo.azc.uam.mx; Fuentes, G.A. [Universidad Autonoma Metropolitana-Iztapalapa, Mexico, D.F. (Mexico); Luna, R. [Universidad Autonoma Metropolitana-Azcapotzalco, Mexico, D.F. (Mexico); Salmones, J.; Zeifert, B. [ESIQIE, Instituto Politecnico Nacional, Mexico, D.F. (Mexico)] Vazquez, A. [Instituto Mexicano del Petroleo, Mexico, D.F. (Mexico)

    2009-09-15

    To produce H{sub 2} from bio-ethanol, the synthesis, characterization and reaction of Pt catalysts exchanged with hydrotalcite were studied. The catalysts obtained were characterized with BET area, x-ray diffraction and Raman, Infrared and UV-vis spectroscopies. The catalytic evaluation was performed with micro-reaction equipment using a water/ethanol ratio of 4 at 45 degrees Celsius. The effect of the W contents was from 0.5 to 3%. X-ray diffraction of the Co and Ni series showed a continuous decrease in crystallinity as W contents increased. Findings from N{sub 2} adsorption show pores in the form of parallel plates and a mesoporous distribution (bimodal) with areas between 151-257 m{sup 2}/g. OH, H{sub 2}O, Al-OH, Mg-OH, W-O and CO32- vibrations and W-O-W surface bonds were observed using infrared and Raman spectroscopy. Tungsten oxide groups were found with UV-vis spectroscopy. The catalyst with the greatest selectivity and stability is between 0.5 and 1% of W, and the highest stability is after 7 h of reaction. In this Pt series, the reaction that most consumed ethanol was that which produces CH{sub 4} and CO{sub 2}. The total conversion increased in function of W contents, between 0.5 and 3%. W stabilized the Pt/hydrotalcite catalyst with 0.5%W being the optimal concentration. The least amount of C{sub 2}H{sub 4} production and no CO was found for this Pt catalyst. [Spanish] Para la produccion de H{sub 2} se estudio la sintesis, caracterizacion y reaccion de catalizadores de Pt intercambiados con hidrotalcita, a partir de bioetanol. Los catalizadores obtenidos se caracterizaron por: area BET, difraccion de rayos X, espectroscopias: Raman, Infrarrojo y UV-vis. La evaluacion catalitica se llevo a cabo en un reactor de lecho fijo usando una relacion agua/etanol de 4 a 450 grados centigrados, se estudio el efecto del contenido de W desde 0.5 hasta 3% en peso. Conforme aumento el contenido de W se encontro por difraccion de rayos X un aumento de la cristalinidad

  17. Efficient method for the conversion of agricultural waste into sugar alcohols over supported bimetallic catalysts.

    Science.gov (United States)

    Tathod, Anup P; Dhepe, Paresh L

    2015-02-01

    Promoter effect of Sn in the PtSn/γ-Al2O3 (AL) and PtSn/C bimetallic catalysts is studied for the conversion of variety of substrates such as, C5 sugars (xylose, arabinose), C6 sugars (glucose, fructose, galactose), hemicelluloses (xylan, arabinogalactan), inulin and agricultural wastes (bagasse, rice husk, wheat straw) into sugar alcohols (sorbitol, mannitol, xylitol, arabitol, galactitol). In all the reactions, PtSn/AL showed enhanced yields of sugar alcohols by 1.5-3 times than Pt/AL. Compared to C, AL supported bimetallic catalysts showed prominent enhancement in the yields of sugar alcohols. Bimetallic catalysts characterized by X-ray diffraction study revealed the stability of catalyst and absence of alloy formation thereby indicating that Pt and Sn are present as individual particles in PtSn/AL. The TEM analysis also confirmed stability of the catalysts and XPS study disclosed formation of electron deficient Sn species which helps in polarizing carbonyl bond to achieve enhanced hydrogenation activity. Copyright © 2014 Elsevier Ltd. All rights reserved.

  18. Dodecahedral W@WC Composite as Efficient Catalyst for Hydrogen Evolution and Nitrobenzene Reduction Reactions.

    Science.gov (United States)

    Chen, Zhao-Yang; Duan, Long-Fa; Sheng, Tian; Lin, Xiao; Chen, Ya-Feng; Chu, You-Qun; Sun, Shi-Gang; Lin, Wen-Feng

    2017-06-21

    Core-shell composites with strong phase-phase contact could provide an incentive for catalytic activity. A simple, yet efficient, H 2 O-mediated method has been developed to synthesize a mesoscopic core-shell W@WC architecture with a dodecahedral microstructure, via a one-pot reaction. The H 2 O plays an important role in the resistance of carbon diffusion, resulting in the formation of the W core and W-terminated WC shell. Density functional theory (DFT) calculations reveal that adding W as core reduced the oxygen adsorption energy and provided the W-terminated WC surface. The W@WC exhibits significant electrocatalytic activities toward hydrogen evolution and nitrobenzene electroreduction reactions, which are comparable to those found for commercial Pt/C, and substantially higher than those found for meso- and nano-WC materials. The experimental results were explained by DFT calculations based on the energy profiles in the hydrogen evolution reactions over WC, W@WC, and Pt model surfaces. The W@WC also shows a high thermal stability and thus may serve as a promising more economical alternative to Pt catalysts in these important energy conversion and environmental protection applications. The current approach can also be extended or adapted to various metals and carbides, allowing for the design and fabrication of a wide range of catalytic and other multifunctional composites.

  19. The atomistic origin of the extraordinary oxygen reduction activity of Pt3Ni7 fuel cell catalysts.

    Science.gov (United States)

    Fortunelli, Alessandro; Goddard Iii, William A; Sementa, Luca; Barcaro, Giovanni; Negreiros, Fabio R; Jaramillo-Botero, Andrés

    2015-07-01

    Recently Debe et al. reported that Pt 3 Ni 7 leads to extraordinary Oxygen Reduction Reaction (ORR) activity. However, several reports show that hardly any Ni remains in the layers of the catalysts close to the surface ("Pt-skin effect"). This paradox that Ni is essential to the high catalytic activity with the peak ORR activity at Pt 3 Ni 7 while little or no Ni remains close to the surface is explained here using large-scale first-principles-based simulations. We make the radical assumption that processing Pt-Ni catalysts under ORR conditions would leach out all Ni accessible to the solvent. To simulate this process we use the ReaxFF reactive force field, starting with random alloy particles ranging from 50% Ni to 90% Ni and containing up to ∼300 000 atoms, deleting the Ni atoms, and equilibrating the resulting structures. We find that the Pt 3 Ni 7 case and a final particle radius around 7.5 nm lead to internal voids in communication with the exterior, doubling the external surface footprint, in fair agreement with experiment. Then we examine the surface character of these nanoporous systems and find that a prominent feature in the surface of the de-alloyed particles is a rhombic structure involving 4 surface atoms which is crystalline-like but under-coordinated. Using density-functional theory, we calculate the energy barriers of ORR steps on Pt nanoporous catalysts, focusing on the O ad -hydration reaction (O ad + H 2 O ad → OH ad + OH ad ) but including the barriers of O 2 dissociation (O 2ad → O ad + O ad ) and water formation (OH ad + H ad → H 2 O ad ). We find that the reaction barrier for the O ad -hydration rate-determining-step is reduced significantly on the de-alloyed surface sites compared to Pt(111). Moreover we find that these active sites are prevalent on the surface of particles de-alloyed from a Pt-Ni 30 : 70 initial composition. These simulations explain the peak in surface reactivity at Pt 3 Ni 7 , and provide a rational guide to

  20. Surface properties and catalytic performance of Pt/LaSrCoO4 catalysts in the oxidation of hexane

    Directory of Open Access Journals (Sweden)

    Hua Zhong

    2007-08-01

    Full Text Available Perovskite-type La2 –xSrxCoO4 mixed oxides have been prepared by calcination at various temperatures of precipitates obtained from aqueous solutions in the presence of citric or ethylenediamintetraacetic (EDTA acids, and have been studied by X-ray diffraction (XRD, surface area (BET measurements, temperature programmed desorption (TPD, temperature programmed reduction (TPR and X-ray photoelectron spectroscopy (XPS. These oxides are catalysts for hexane oxidation, with the greatest activity for LaSrCoO4 calcined at 750 C. This has extensive oxygen vacancies and large internal surface area. Pt-modified LaSrCoO4 catalysts are significantly more active than the Pt-free system. Both surface and bulk phases of the preovskitetype oxides contribute to hexane oxidation.

  1. Fine platinum nanoparticles supported on a porous ceramic membrane as efficient catalysts for the removal of benzene.

    Science.gov (United States)

    Liu, Hui; Li, Chengyin; Ren, Xiaoyong; Liu, Kaiqi; Yang, Jun

    2017-11-29

    It would be desirable to remove volatile organic compounds (VOCs) while we eliminate the dusts using silicon carbide (SiC)-based porous ceramics from the hot gases. Aiming at functionalizing SiC-based porous ceramics with catalytic capability, we herein report a facile strategy to integrate high efficient catalysts into the porous SiC substrates for the VOC removal. We demonstrate an aqueous salt method for uniformly distributing fine platinum (Pt) particles on the alumina (Al 2 O 3 ) layers, which are pre-coated on the SiC substrates as supports for VOC catalysts. We confirm that at a Pt mass loading as low as 0.176% and a weight hourly space velocity of 6000 mL g -1 h -1 , the as-prepared Pt/SiC@Al 2 O 3 catalysts can convert 90% benzene at a temperature of ca. 215 °C. The results suggest a promising way to design ceramics-based bi-functional materials for simultaneously eliminating dusts and harmful VOCs from various hot gases.

  2. Catalytic Performance for Hydrocarbon Production from Syngas on the Promoted Co-Based Hybrid Catalysts; Influence of Pt Contents

    Directory of Open Access Journals (Sweden)

    Suk-Hwan Kang

    2017-10-01

    How to Cite: Kang, S.H., Ryu, J.H., Kim, J.H., Kim, H.S., Yang, H.C., Chung, D.Y. (2017. Catalytic Performance for Hydrocarbon Production from Syngas on the Promoted Co-Based Hybrid Catalysts; Influence of Pt Contents. Bulletin of Chemical Reaction Engineering & Catalysis, 12 (3: 452-459 (doi:10.9767/bcrec.12.3.592.452-459

  3. First principles study of (Cd, Hg, In, Tl, Sn, Pb, As, Sb, Bi, Se) modified Pt(111), Pt(100) and Pt(211) electrodes as CO oxidation catalysts

    DEFF Research Database (Denmark)

    Tripkovic, Vladimir

    2015-01-01

    . The coverage dependence as a function of potential for ten different adatom species (Cd, Hg, In, Tl, Sn, Pb, As, Sb, Bi, Se) on bare and CO saturated Pt(111), Pt(100) and Pt(211) surfaces has been established by means of Density Functional Theory calculations. Most of the adatoms are very stable under standard......, given by the OH formation potentials from water, is dependent on the oxophilicity of the adatoms, and is found to scale almost inversely with the adatom stability. In electrolyte solutions saturated with CO, the stability reduces to roughly half of that on bare Pt surfaces. Irrespective of the CO...

  4. Systematic Investigations of the Oxygen Reduction Reaction on Pt Based Catalysts Comparing Transient and Steady State Performance

    DEFF Research Database (Denmark)

    Deng, Yujia

    . Above 0.6 VRHE, OHad begins to form on the surface and at0.95 VRHE a monolayer completes. Above 0.95 VRHE, OHad can be oxidized to Oad and at 1.1VRHE a monolayer of Oad is formed. When the potential increases further above 1.1 VRHE, Pt-oxidestarts to form. The ORR can only proceed on free Pt sites...... the electrode potential is held. A combination of a site blockingmechanism and an increase in viscosity at the polarized electrode surface is proposed toexplain this extraordinary behavior in H3PO4.Atomic layer deposition of Pt onto an Au substrate is employed as model catalyst toinvestigate how ligand...

  5. Design of bimetal catalysts Pt-Ni/CeO_2-1D for generation of H_2 by the reforming reaction of methanol

    International Nuclear Information System (INIS)

    Sarmiento F, I.

    2016-01-01

    CeO_2 nano rods were synthesized by hydrothermal method and were used as support for preparing catalysts bimetallic Pt Ni / CeO_2-1D. The catalysts were prepared by classical impregnation by the conventional wet method. The prepared catalysts are Pt (0.5 %) - Ni (5 %) / CeO_2 and Pt (0.5 %) - Ni (15 %) / CeO_2, which were characterized by different physico-chemical techniques: Bet, Sem, TPR and XRD, that were evaluated in the Auto thermal Steam reforming of Methanol for H_2 production. The Bet surface area results, show that the surface area of the catalysts decreases as the nominal load of Ni in the catalyst, increases. Sem shows, that the catalyst support (CeO_2-1D) and the bimetallic catalysts are conformed by nano rods. By XRD were identified the crystalline phases present, in the catalytic material: cerianite distinctive phase of cerium oxide and metallic Ni; however it was not possible to observe diffraction peaks of Platinum using this technique. The temperature-programmed reduction (TPR) analysis allowed to obtain the reduction profiles, of the different species present on the catalysts. The catalytic activity tests carried out, showed that the catalysts total 100% methanol conversion is achieved at 300 degrees Celsius, making them excellent, to be used in reactions at low temperature conditions. Selectivity towards H_2, is very similar in both catalysts, and it reaches a 50% yield per mole of methanol fed stoichiometrically. (Author)

  6. Electrochemical characterization of Pt-CeO{sub 2}/C and Pt-Ce{sub x}Zr{sub 1-x}O{sub 2}/C catalysts for ethanol electro-oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Bai, Yuxia; Qiu, Xinping; Xi, Jingyu; Wang, Jianshe; Li, Jinfeng; Zhu, Wentao; Chen, Liquan [Key Laboratory of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing 100084 (China); Wu, Jianjun [Key Laboratory of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing 100084 (China); Department of Chemistry, Shijiazhuang College, Shijiazhuang 050801 (China)

    2007-04-24

    Pt-CeO{sub 2}/C and a series of Pt-Ce{sub x}Zr{sub 1-x}O{sub 2}/C catalyst powders with different Ce/Zr ratio were prepared and evaluated in terms of the electrochemical activity for ethanol electro-oxidation using cyclic voltammetry (CV), steady state polarization experiments and CO-stripping technique at room temperature. XRD results show that Ce{sub x}Zr{sub 1-x}O{sub 2} and Pt coexist in the Pt-Ce{sub x}Zr{sub 1-x}O{sub 2}/C catalyst and Ce{sub x}Zr{sub 1-x}O{sub 2} has no effect on the crystalline lattice of Pt. TEM results show that the Pt and Ce{sub x}Zr{sub 1-x}O{sub 2} particles dispersed uniformly over the surface of the carbon black. Cyclic voltammetry results show that the mass activity and specific activity of Pt-CeO{sub 2}/C for ethanol electro-oxidation is higher than that of Pt/C. The structure and Ce/Zr ratio of Pt-Ce{sub x}Zr{sub 1-x}O{sub 2}/C has effect on the catalytic activity of catalysts. CO-stripping voltammetry showed that the inclusion of CeO{sub 2} and Ce{sub x}Zr{sub 1-x}O{sub 2} favors the CO oxidation at lower potential. (author)

  7. An anodic alumina supported Ni-Pt bimetallic plate-type catalysts for multi-reforming of methane, kerosene and ethanol

    KAUST Repository

    Zhou, Lu; Guo, Yu; Kameyama, Hideo; Basset, Jean-Marie

    2014-01-01

    . The prepared Ni-Pt catalyst showed excellent performance during steam reforming of methane, kerosene and ethanol under both 3000 h stationary and 500-time daily start-up and shut-down operation modes. Self-activation ability of this catalyst was evidenced

  8. Unusual attempt to direct the growth of bimetallic Ag@Pt nanorods on electrochemically reduced graphene oxide nanosheets by electroless exchange of Cu by Pt for an efficient alcohol oxidation

    Science.gov (United States)

    Jeena, S. E.; Gnanaprakasam, P.; Selvaraju, T.

    2017-01-01

    A simple and an efficient tool for the direct growth of bimetallic Ag@Pt nanorods (NRDs) on electrochemically reduced graphene oxide (ERGO) nanosheets was developed at glassy carbon electrode (GCE). Initially, Cu shell was grown on Ag core as Ag@Cu NRD by the seed-mediated growth method. Accordingly, Cu shell has been successfully replaced by Pt using the electroless galvanic replacement method with ease by effective functionalization of L-tryptophan on ERGO surface (L-ERGO), which eventually plays an important role in the direct growth of one-dimensional bimetallic NRDs. As a result, the synthesized Ag@Pt NRD-supported L-ERGO nanosheets (Ag@Pt NRDs/L-ERGO/GCE) were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), energy-dispersive X-ray analysis (EDAX) and Raman spectroscopy. Anodic stripping voltammetry was used to explore its electrochemical properties. Finally, the developed bimetallic Ag@Pt NRDs/L-ERGO/GCEs were studied as a better electrocatalyst compared to the commercial catalysts such as Pt40/C or Pt20/C-loaded electrode for the oxidation of ethanol or methanol with a high tolerance level and an enhanced current density. In addition, the long-term stability was studied using chronoamperometry for 1000 s at the bimetallic NRD electrode for alcohol oxidation which impedes the fouling properties. The unfavourable and favourable electrooxidation of ethanol at Ag@Cu NRDs/L-ERGO/GCE (a) and Ag@Pt NRDs/L-ERGO/GCE (b) is discussed. The synergistic effect of Ag core and catalytic properties of Pt shell at Ag@Pt NRDs/L-ERGO/GCE tend to strongly minimize the CO poisoning effect and enhanced ethanol electrooxidation.

  9. Unusual attempt to direct the growth of bimetallic Ag@Pt nanorods on electrochemically reduced graphene oxide nanosheets by electroless exchange of Cu by Pt for an efficient alcohol oxidation

    International Nuclear Information System (INIS)

    Jeena, S. E.; Gnanaprakasam, P.; Selvaraju, T.

    2017-01-01

    A simple and an efficient tool for the direct growth of bimetallic Ag@Pt nanorods (NRDs) on electrochemically reduced graphene oxide (ERGO) nanosheets was developed at glassy carbon electrode (GCE). Initially, Cu shell was grown on Ag core as Ag@Cu NRD by the seed-mediated growth method. Accordingly, Cu shell has been successfully replaced by Pt using the electroless galvanic replacement method with ease by effective functionalization of L-tryptophan on ERGO surface (L-ERGO), which eventually plays an important role in the direct growth of one-dimensional bimetallic NRDs. As a result, the synthesized Ag@Pt NRD-supported L-ERGO nanosheets (Ag@Pt NRDs/L-ERGO/GCE) were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), energy-dispersive X-ray analysis (EDAX) and Raman spectroscopy. Anodic stripping voltammetry was used to explore its electrochemical properties. Finally, the developed bimetallic Ag@Pt NRDs/L-ERGO/GCEs were studied as a better electrocatalyst compared to the commercial catalysts such as Pt_4_0/C or Pt_2_0/C-loaded electrode for the oxidation of ethanol or methanol with a high tolerance level and an enhanced current density. In addition, the long-term stability was studied using chronoamperometry for 1000 s at the bimetallic NRD electrode for alcohol oxidation which impedes the fouling properties. The unfavourable and favourable electrooxidation of ethanol at Ag@Cu NRDs/L-ERGO/GCE (a) and Ag@Pt NRDs/L-ERGO/GCE (b) is discussed. The synergistic effect of Ag core and catalytic properties of Pt shell at Ag@Pt NRDs/L-ERGO/GCE tend to strongly minimize the CO poisoning effect and enhanced ethanol electrooxidation.

  10. Unusual attempt to direct the growth of bimetallic Ag@Pt nanorods on electrochemically reduced graphene oxide nanosheets by electroless exchange of Cu by Pt for an efficient alcohol oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Jeena, S. E.; Gnanaprakasam, P. [Karunya University, Department of Chemistry (India); Selvaraju, T., E-mail: veluselvaraju@gmail.com [Bharathiar University, Department of Chemistry (India)

    2017-01-15

    A simple and an efficient tool for the direct growth of bimetallic Ag@Pt nanorods (NRDs) on electrochemically reduced graphene oxide (ERGO) nanosheets was developed at glassy carbon electrode (GCE). Initially, Cu shell was grown on Ag core as Ag@Cu NRD by the seed-mediated growth method. Accordingly, Cu shell has been successfully replaced by Pt using the electroless galvanic replacement method with ease by effective functionalization of L-tryptophan on ERGO surface (L-ERGO), which eventually plays an important role in the direct growth of one-dimensional bimetallic NRDs. As a result, the synthesized Ag@Pt NRD-supported L-ERGO nanosheets (Ag@Pt NRDs/L-ERGO/GCE) were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), energy-dispersive X-ray analysis (EDAX) and Raman spectroscopy. Anodic stripping voltammetry was used to explore its electrochemical properties. Finally, the developed bimetallic Ag@Pt NRDs/L-ERGO/GCEs were studied as a better electrocatalyst compared to the commercial catalysts such as Pt{sub 40}/C or Pt{sub 20}/C-loaded electrode for the oxidation of ethanol or methanol with a high tolerance level and an enhanced current density. In addition, the long-term stability was studied using chronoamperometry for 1000 s at the bimetallic NRD electrode for alcohol oxidation which impedes the fouling properties. The unfavourable and favourable electrooxidation of ethanol at Ag@Cu NRDs/L-ERGO/GCE (a) and Ag@Pt NRDs/L-ERGO/GCE (b) is discussed. The synergistic effect of Ag core and catalytic properties of Pt shell at Ag@Pt NRDs/L-ERGO/GCE tend to strongly minimize the CO poisoning effect and enhanced ethanol electrooxidation.

  11. Pt nanoparticles residing in the pores of porous LaNiO₃ nanocubes as high-efficiency electrocatalyst for direct methanol fuel cells.

    Science.gov (United States)

    Yu, Nan; Kuai, Long; Wang, Qing; Geng, Baoyou

    2012-09-07

    Pt-filled porous LaNiO₃ cubes are prepared through a facile route. The characterizations reveal that large numbers of pores (9-10 nm) are distributed homogeneously in porous LaNiO₃ cubes. The Pt nanoparticles residing in the pores of porous LaNiO₃ cubes are about 5 nm in size. The investigation on the electrocatalytic activity reveals that electrocatalytic activity of the obtained Pt loaded porous LaNiO₃ nanocubes exhibit a significantly improved electrochemical active surface area (EASA) and a remarkably enhanced electrocatalytic performance toward methanol oxidation. The results are significant for improving the efficiency of Pt-based catalysts for DMFCs as well as the applications of perovskite compounds.

  12. Microporous Cokes Formed in Zeolite Catalysts Enable Efficient Solar Evaporation

    KAUST Repository

    Wang, Jianjian

    2017-03-13

    Cokes are inevitably generated during zeolite-catalyzed reactions as deleterious side products that deactivate the catalyst. In this study, we in-situ converted cokes into carbons within the confined microporous zeolite structures and evaluated their performances as absorbing materials for solar-driven water evaporation. With a properly chosen zeolite, the cokederived carbons possessed ordered interconnected pores and tunable compositions. We found that the porous structure and the oxygen content in as-prepared carbons had important influences on their energy conversion efficiencies. Among various investigated carbon materials, the carbon derived from the methanol-to-olefins reaction over zeolite Beta gave the highest conversion efficiency of 72% under simulated sunlight with equivalent solar intensity of 2 suns. This study not only demonstrates the great potential of traditionally useless cokes for solar thermal applications but also provides new insights into the design of carbon-based absorbing materials for efficient solar evaporation.

  13. Pt nanocrystals electrodeposited on reduced graphene oxide/carbon fiber paper with efficient electrocatalytic properties

    Directory of Open Access Journals (Sweden)

    Zhiling Chen

    2017-08-01

    Full Text Available Carbon fiber paper (CFP wrapped with reduced graphene oxide (rGO film as the composite support (rGO/CFP of Pt catalysts was studied. It was found that rGO could affect the size and morphology of Pt nanocrystals (NCs. Concave nanocubes (CNC Pt NCs ~ 20 nm were uniformly electrodeposited on high reduced HrGO/CFP while irregular Pt NCs ~ 62 nm were loaded on low reduced LrGO. Compared with Pt-LrGO/CFP and Pt-MrGO/CFP, the CNC Pt-HrGO/CFP exhibited a higher electrochemically active surface area (121.7 m2 g−1, as well as enhanced electrooxidation activity of methanol (499 mA mg−1 and formic acid (950 mA mg−1. The results further demonstrated that the CNC Pt-HrGO/CFP could serve as the gas diffusion electrode in fuel cells and yielded a satisfactory performance (1855 mW mg−1. The work can provide an attractive perspective on the convenient preparation of the novel gas diffusion electrode for proton exchange membrane fuel cells.

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

    Science.gov (United States)

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

    2016-02-01

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

  15. Phosphate-Doped Carbon Black as Pt Catalyst Support: Co-catalytic Functionality for Dimethyl Ether and Methanol Electro-oxidation

    DEFF Research Database (Denmark)

    Yin, Min; Huang, Yunjie; Li, Qingfeng

    2014-01-01

    ). The supported Pt catalysts show significant improvement in catalytic activity towards the direct oxidation of methanol and DME, attributable to the enhanced adsorption and dehydrogenation of methanol and DME, as well as the presence of activated OH species in the catalysts. The latter is demonstrated......Niobium-phosphate-doped (NbP-doped) carbon blacks were prepared as the composite catalyst support for Pt nanoparticles. Functionalities of the composite include intrinsic proton conductivity, surface acidity, and interfacial synergistic interactions with methanol and dimethyl ether (DME...... to facilitate the removal of CO intermediates formed during the oxidation reactions....

  16. Sulfur-tolerant Pt-supported catalysts for benzene hydrogenation. II. Influence of cation exchange level for Pt/MOR-based catalysts

    NARCIS (Netherlands)

    Simon, L.; van Ommen, J.G.; Jentys, A.; Lercher, J.A.

    2001-01-01

    Two reaction pathways are described for the hydrogenation of benzene over Pt/MOR, i.e., (i) on the metal particles and (ii) on Brønsted acid sites of MOR at the boundary to the metal, with atomic hydrogen being dissociated on the metal. The ratio between the two pathways depends on the zeolite acid

  17. Pt{sub 1-x}Co{sub x} nanoparticles as cathode catalyst for proton exchange membrane fuel cells with enhanced catalytic activity

    Energy Technology Data Exchange (ETDEWEB)

    Wu Huimin; Wexler, David; Liu Huakun [Institute for Superconducting and Electronic Materials, School of Mechanical, Materials and Mechatronics Engineering, University of Wollongong, Wollongong, NSW 2522 (Australia); Savadogo, O. [Materials Engineering Department, Ecole Polytechique de Montreal, Montreal, QC H3C3A7 (Canada); Ahn, Jungho [Department of Materials Engineering, Andong National University, Andong (Korea, Republic of); Wang Guoxiu, E-mail: Guoxiu.Wang@uts.edu.au [Department of Chemistry and Forensic Science, University of Technology, Sydney, NSW 2007 (Australia)

    2010-11-01

    Nanosize carbon-supported Pt{sub 1-x}Co{sub x} (x = 0.2, 0.3, and 0.45) electrocatalysts were prepared by a chemical reduction method using sodium borohydride (NaBH{sub 4}) as the reduction agent. Transmission electron microscopy examination showed uniform dispersion of Pt{sub 1-x}Co{sub x} alloy catalysts on carbon matrix, with the particle size less than 10 nm. The electrochemical characteristics of Pt{sub 1-x}Co{sub x} alloy catalysts were studied by cyclic voltammetry, linear sweep voltammetry, and chronoamperometric testing. The as-prepared Pt{sub 1-x}Co{sub x} alloy nanoparticles could be promising cathode catalysts for oxygen reduction in proton exchange membrane fuel cells with the feature of much reduced cost, but significantly increased catalytic activity.

  18. Electrodeposited Pt for cost-efficient and flexible dye-sensitized solar cells

    International Nuclear Information System (INIS)

    Kim, Seok-Soon; Nah, Yoon-Chae; Noh, Yong-Young; Jo, Jang; Kim, Dong-Yu

    2006-01-01

    Pt electrodes were prepared by direct and pulse current electrodeposition for use as counter electrodes in dye-sensitized solar cells. Scanning electron microscope and transmission electron microscope images confirmed the formation of uniform Pt nanoclusters of ∼40 nm composed of 3 nm nanoparticles, when the pulse current electrodeposition method was used, as opposed to the dendritic growth of Pt by the results from direct current electrodeposition. By applying pulse electrodeposited Pt which has a 1.86 times higher surface area compared to direct current electrodeposited Pt, short-circuit current and conversion efficiency were increased from 10.34 to 14.11 mA/cm 2 and from 3.68 to 5.03%, respectively. In addition, a flexible solar cell with a pulse current electrodeposited Pt counter electrode with a conversion efficiency of 0.86% was demonstrated

  19. Dry (CO{sub 2}) reforming of methane over Pt catalysts studied by DFT and kinetic modeling

    Energy Technology Data Exchange (ETDEWEB)

    Niu, Juntian [Key Laboratory of Low-grade Energy Utilization Technologies and Systems, Ministry of Education of PRC, Chongqing University, Chongqing, 400044 (China); College of Power Engineering, Chongqing University, Chongqing, 400044 (China); Du, Xuesen, E-mail: xuesendu@cqu.edu.cn [Key Laboratory of Low-grade Energy Utilization Technologies and Systems, Ministry of Education of PRC, Chongqing University, Chongqing, 400044 (China); College of Power Engineering, Chongqing University, Chongqing, 400044 (China); Ran, Jingyu, E-mail: jyran@189.cn [Key Laboratory of Low-grade Energy Utilization Technologies and Systems, Ministry of Education of PRC, Chongqing University, Chongqing, 400044 (China); College of Power Engineering, Chongqing University, Chongqing, 400044 (China); Wang, Ruirui [Key Laboratory of Low-grade Energy Utilization Technologies and Systems, Ministry of Education of PRC, Chongqing University, Chongqing, 400044 (China); College of Power Engineering, Chongqing University, Chongqing, 400044 (China)

    2016-07-15

    Graphical abstract: - Highlights: • CH appears to be the most abundant species on Pt(1 1 1) surface in CH{sub 4} dissociation. • CO{sub 2}* + H* → COOH* + * → CO* + OH* is the dominant reaction pathway in CO{sub 2} activation. • Major reaction pathway in CH oxidation: CH* + OH* → CHOH* + * → CHO* + H* → CO* + 2H*. • C* + OH* → COH* + * → CO* + H* is the dominant reaction pathway in C oxidation. - Abstract: Dry reforming of methane (DRM) is a well-studied reaction that is of both scientific and industrial importance. In order to design catalysts that minimize the deactivation and improve the selectivity and activity for a high H{sub 2}/CO yield, it is necessary to understand the elementary reaction steps involved in activation and conversion of CO{sub 2} and CH{sub 4}. In our present work, a microkinetic model based on density functional theory (DFT) calculations is applied to explore the reaction mechanism for methane dry reforming on Pt catalysts. The adsorption energies of the reactants, intermediates and products, and the activation barriers for the elementary reactions involved in the DRM process are calculated over the Pt(1 1 1) surface. In the process of CH{sub 4} direct dissociation, the kinetic results show that CH dissociative adsorption on Pt(1 1 1) surface is the rate-determining step. CH appears to be the most abundant species on the Pt(1 1 1) surface, suggesting that carbon deposition is not easy to form in CH{sub 4} dehydrogenation on Pt(1 1 1) surface. In the process of CO{sub 2} activation, three possible reaction pathways are considered to contribute to the CO{sub 2} decomposition: (I) CO{sub 2}* + * → CO* + O*; (II) CO{sub 2}* + H* → COOH* + * → CO* + OH*; (III) CO{sub 2}* + H* → mono-HCOO* + * → bi-HCOO* + * [CO{sub 2}* + H* → bi-HCOO* + *] → CHO* + O*. Path I requires process to overcome the activation barrier of 1.809 eV and the forward reaction is calculated to be strongly endothermic by 1.430 eV. In

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

    Science.gov (United States)

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

    2017-06-01

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

  1. Deoxygenation of Palmitic and Lauric Acids over Pt/ZIF-67 Membrane/Zeolite 5A Bead Catalysts.

    Science.gov (United States)

    Yang, Liqiu; Carreon, Moises A

    2017-09-20

    The deoxygenation of palmitic and lauric acids over 0.5 wt % Pt/ZIF-67 membrane/zeolite 5A bead catalysts is demonstrated. Almost complete conversion (% deoxygenation of ≥95%) of these two fatty acids was observed over both fresh and recycled catalyst after a 2 h reaction time. The catalysts displayed high selectivity to pentadecane and undecane via decarboxylation reaction pathway even at low 0.5 wt % Pt loading. Selectivity to pentadecane and undecane as high as ∼92% and ∼94% was observed under CO 2 atmosphere when palmitic and lauric acids were used respectively as reactants. Depending on the reaction gas atmosphere, two distinctive reaction pathways were observed: decarboxylation and hydrodeoxygenation. Specifically, it was found that decarboxylation reaction pathway was more favorable in the presence of helium and CO 2 , while hydrodeoxygenation pathway strongly competed against the decarboxylation pathway when hydrogen was employed during the deoxygenation reactions. Esters were identified as the key reaction intermediates leading to decarboxylation and hydrodeoxygenation pathways.

  2. Exploring the Potential of Different-Sized Supported Subnanometer Pt Clusters as Catalysts for Wet Chemical Applications

    KAUST Repository

    Rondelli, Manuel

    2017-05-10

    The use of physicochemical preparation techniques of metal clusters in the ultrahigh vacuum (UHV) allows for high control of cluster nuclearity and size distribution for fundamental studies in catalysis. Surprisingly, the potential of these systems as catalysts for organic chemistry transformations in solution has not been explored. To this end, single Pt atoms and Pt clusters with two narrow size distributions were prepared in the UHV and applied for the hydrogenation of p-chloronitrobenzene to p-chloroaniline in ethanol. Following the observation of very high catalytic turnovers (approaching the million molecules of p-nitroaniline formed per Pt cluster) and of size-dependent activity, this work addresses fundamental questions with respect to the suitability of these systems as heterogeneous catalysts for the conversion of solution-phase reagents. For this purpose, we employ scanning transmission electron microscopy (STEM) and X-ray photoelectron spectroscopy (XPS) characterization before and after reaction to assess the stability of the clusters on the support and the question of heterogeneity versus homogeneity in the catalytic process.

  3. Balance of Nanostructure and Bimetallic Interactions in Pt Model Fuel Cell Catalysts

    DEFF Research Database (Denmark)

    Friebel, Daniel; Viswanathan, Venkatasubramanian; Miller, Daniel J.

    2012-01-01

    We have studied the effect of nanostructuring in Pt monolayer model electrocatalysts on a Rh(111) single-crystal substrate on the adsorption strength of chemisorbed species. In situ high energy resolution fluorescence detection X-ray absorption spectroscopy at the Pt L3 edge reveals characteristic...... changes of the shape and intensity of the “white-line” due to chemisorption of atomic hydrogen (Had) at low potentials and oxygen-containing species (O/OHad) at high potentials. On a uniform, two-dimensional Pt monolayer grown by Pt evaporation in ultrahigh vacuum, we observe a significant destabilization...... of both Had and O/OHad due to strain and ligand effects induced by the underlying Rh(111) substrate. When Pt is deposited via a wet-chemical route, by contrast, three-dimensional Pt islands are formed. In this case, strain and Rh ligand effects are balanced with higher local thickness of the Pt islands...

  4. Preparation of ternary Pt/Rh/SnO2 anode catalysts for use in direct ethanol fuel cells and their electrocatalytic activity for ethanol oxidation reaction

    Science.gov (United States)

    Higuchi, Eiji; Takase, Tomonori; Chiku, Masanobu; Inoue, Hiroshi

    2014-10-01

    Pt, Rh and SnO2 nanoparticle-loaded carbon black (Pt/Rh/SnO2/CB) catalysts with different contents of Pt and Rh were prepared by the modified Bönnemann method. The mean size and size distribution of Pt, Rh and SnO2 for Pt-71/Rh-4/SnO2/CB (Pt : Rh : Sn = 71 at.%: 4 at.%: 25 at.%) were 3.8 ± 0.7, 3.2 ± 0.7 and 2.6 ± 0.5 nm, respectively, indicating that Pt, Rh and SnO2 were all nanoparticles. The onset potential of ethanol oxidation current for the Pt-65/Rh-10/SnO2/CB and Pt-56/Rh-19/SnO2/CB electrodes was ca. 0.2 V vs. RHE which was ca. 0.2 V less positive than that for the Pt/CB electrode. The oxidation current at 0.6 V for the Pt/Rh/SnO2/CB electrode (ca. 2% h-1) decayed more slowly than that at the Pt/SnO2/CB electrode (ca. 5% h-1), indicating that the former was superior in durability to the latter. The main product of EOR in potentiostatic electrolysis at 0.6 V for the Pt-71/Rh-4/SnO2/CB electrode was acetic acid.

  5. Study on Pt-structured anodic alumina catalysts for catalytic combustion of toluene: Effects of competitive adsorbents and competitive impregnation methods

    Science.gov (United States)

    Zhang, Qi; Luan, Hongjuan; Li, Tao; Wu, Yongqiang; Ni, Yanhui

    2016-01-01

    Novel competitive impregnation methods were used to prepare high dispersion Pt-structured anodic alumina catalysts. It is found that competitive adsorbents owning different acidity result in different Pt loading amount and also exert great effects on Pt distribution, particle size and redox ability. The suitable adsorption ability of lactic acid led to its best activity for catalytic combustion of toluene. Co-competitive and pre-competitive impregnation methods were also compared and the mechanisms of two competitive methods were proposed. Co-competitive impregnation made Pt distribute more uniformly through pore channels and resulted in better catalytic activity, because of the weaker spatial constraint effect of lactic acid. Furthermore, the optimized Pt-structured anodic alumina catalyst also showed a good chlorine-resistance under moisture atmosphere, because water could promote the reaction of dichloromethane (DCM) transformation and clean chloride by-products to release more active sites.

  6. The Study on the Performance of Carbon Supported PtSnM (M = W, Pd, and Ni) Ternary Electro-Catalysts for Ethanol Electro-Oxidation Reaction.

    Science.gov (United States)

    Noh, Chang Soo; Heo, Dong Hyun; Lee, Ki Rak; Jeon, Min Ku; Sohn, Jung Min

    2016-05-01

    PtSn/C and Pt5Sn4M/C (M = W, Pd, Ni) electrocatalysts were prepared by impregnation method using NaBH4 as a reducing agent. Chemical composition, crystalline size, and alloy formation were determined by EDX, XRD and TEM. The average particle sizes of the synthesized catalysts were approximately 3.64-4.95 nm. The electro-chemical properties were measured by CO stripping, cyclic voltammetry, linear sweep voltammetry, and chronoamperometry. The maximum specific activity of the electro-catalysts for ethanol electro-oxidation was 406.08 mA m(-2) in Pt5Sn4Pd/C. The poisoning rate of the Pt5Sn4Pd/C (0.0017% s(-1)) was 4.5 times lower than that of the PtSn/C (0.0076% s(-1)).

  7. Investigation of the promoting effect of Mn on a Pt/C catalyst for the steam and aqueous phase reforming of glycerol

    Energy Technology Data Exchange (ETDEWEB)

    Bossola, Filippo; Pereira-Hernández, Xavier Isidro; Evangelisti, Claudio; Wang, Yong; Dal Santo, Vladimiro

    2017-05-01

    The catalytic performances in steam reforming (SR) and aqueous phase reforming (APR) of glycerol of a bimetallic Pt-Mn catalyst supported on activated carbon are investigated and correlated with the surface properties of the catalyst. Under SR conditions, Mn showed a significant promoting effect over Pt/C, both in terms of hydrogen production rate and conversion, with a higher selectivity toward the glycerol dehydration products. Upon addition of Mn the amount of strong Lewis acid sites increased, promoting the dehydration of glycerol and favoring the CAO over CAC cleavage at expenses of hydrogen selectivity. Conversely, under APR conditions, a slightly higher hydrogen selectivity and only minimal enhancement in hydrogen production were found, while the products selectivity was comparable to Pt/C. Most of Mn leached into the aqueous media, but the remaining (<5% of the fresh parent sample) might be alloyed with Pt and promote the CO desorption from neighbor Pt sites.

  8. Carbon-supported ternary PtSnIr catalysts for direct ethanol fuel cell

    Energy Technology Data Exchange (ETDEWEB)

    Ribeiro, J.; Kokoh, K.B.; Coutanceau, C.; Leger, J.-M. [Equipe Electrocatalyse, UMR 6503 CNRS, Universite de Poitiers, 40 avenue du Recteur Pineau 86022 Poitiers Cedex (France); Dos Anjos, D.M. [Equipe Electrocatalyse, UMR 6503 CNRS, Universite de Poitiers, 40 avenue du Recteur Pineau 86022 Poitiers Cedex (France); Instituto de Quimica de Sao Carlos, Universidade de Sao Paulo, Caixa Postal 780, 13560-970 Sao Carlos, SP (Brazil); Olivi, P.; De Andrade, A.R. [Departamento de Quimica da Faculdade de Filosofia, Ciencias e Letras de Ribeirao Preto, Universidade de Sao Paulo, Av. Bandeirantes, 3900, 14040-901 Ribeirao Preto, SP (Brazil); Tremiliosi-Filho, G. [Instituto de Quimica de Sao Carlos, Universidade de Sao Paulo, Caixa Postal 780, 13560-970 Sao Carlos, SP (Brazil)

    2007-08-01

    Binary PtIr, PtSn and ternary PtSnIr electrocatalysts were prepared by the Pechini-Adams modified method on carbon Vulcan XC-72, and these materials were characterized by TEM and XRD. The XRD results showed that the electrocatalysts consisted of the Pt displaced phase, suggesting the formation of solid solutions between the metals Pt/Ir and Pt/Sn. However, the increase in Sn loading promoted phase separation, with the formation of peaks typical of cubic Pt{sub 3}Sn. The electrochemical investigation of these different electrode materials was carried out as a function of the electrocatalyst composition, in a 0.5 mol dm{sup -3} H{sub 2}SO{sub 4} solution, with either the presence or the absence of ethanol. Cyclic voltammetric measurements and chronoamperometric results obtained at room temperature showed that PtSn/C and PtSnIr/C displayed better electrocatalytic activity for ethanol electrooxidation compared to PtIr/C and Pt/C, mainly at low potentials. The oxidation process was also investigated by in situ infrared reflectance spectroscopy, to identify the adsorbed species. Linearly adsorbed CO and CO{sub 2} were found, indicating that the cleavage of the C-C bond in the ethanol substrate occurred during the oxidation process. At 90 C, the Pt{sub 89}Sn{sub 11}/C and Pt{sub 68}Sn{sub 9}Ir{sub 23}/C electrocatalysts displayed higher current and power performances as anode materials in a direct ethanol fuel cell (DEFC). (author)

  9. Fabrication of Highly Stable and Efficient PtCu Alloy Nanoparticles on Highly Porous Carbon for Direct Methanol Fuel Cells.

    Science.gov (United States)

    Khan, Inayat Ali; Qian, Yuhong; Badshah, Amin; Zhao, Dan; Nadeem, Muhammad Arif

    2016-08-17

    Boosting the durability of Pt nanoparticles by controlling the composition and morphology is extremely important for fuel cells commercialization. We deposit the Pt-Cu alloy nanoparticles over high surface area carbon in different metallic molar ratios and optimize the conditions to achieve desired material. The novel bimetallic electro-catalyst {Pt-Cu/PC-950 (15:15%)} offers exceptional electrocatalytic activity when tested for both oxygen reduction reaction and methanol oxidation reactions. A high mass activity of 0.043 mA/μgPt (based on Pt mass) is recorded for ORR. An outstanding longevity of this electro-catalyst is noticed when compared to 20 wt % Pt loaded either on PC-950 or commercial carbon. The high surface area carbon support offers enhanced activity and prevents the nanoparticles from agglomeration, migration, and dissolution as evident by TEM analysis.

  10. Kinetic study of methanol oxidation on Pt2Ru3/C catalyst in the alkaline media

    Directory of Open Access Journals (Sweden)

    A. V. TRIPKOVIC

    2007-11-01

    Full Text Available The interaction of acridine orange (AO with double-stranded (ds The electrochemical oxidation of methanol in NaOH solution was examined on a thin film Pt2Ru3/C electrode. The XRD pattern revealed that the Pt2Ru3 alloy consisted of a solid solution of Ru in Pt and a small amount of Ru or a solid solution of Pt in Ru. It was shown that in alkaline solution, the difference in activity between Pt/C and Pt2Ru3/C is significantly smaller than in acid solution. It is proposed that the reaction follows a quasi bifunctional mechanism. The kinetic parameters indicated that the chemical reaction between adsorbed COad and OHad species could be the rate limiting step.

  11. One-pot solvothermal synthesis of ordered intermetallic Pt{sub 2}In{sub 3} as stable and efficient electrocatalyst towards direct alcohol fuel cell application

    Energy Technology Data Exchange (ETDEWEB)

    Jana, Rajkumar; Peter, Sebastian C., E-mail: sebastiancp@jncasr.ac.in

    2016-10-15

    Ordered intermetallic Pt{sub 2}In{sub 3} nanoparticles have been synthesized by superhydride reduction of K{sub 2}PtCl{sub 4} and InCl{sub 3}.xH{sub 2}O precursors using facile, one-pot solvothermal method. We report surfactant free solvothermal synthesis of a novel ordered Pt{sub 2}In{sub 3} intermetallic nanoparticles for the first time. The structure and morphology of the catalyst has been confirmed by powder X-ray diffraction, transmission electron microscopy, field emission scanning electron microscopy, energy-dispersive spectrometry and X-ray photoelectron spectroscopy. The electrocatalytic properties of the catalysts have been investigated by cyclic voltammetry and chronoamperometry. The as prepared Pt{sub 2}In{sub 3} catalyst exhibit far superior electrocatalytic activity and stability towards alcohol oxidation over commercial Pt/C. The specific activity of as synthesized catalyst was found to be ~3.2 and ~2.3 times higher than commercial Pt/C for methanol and ethanol oxidation, respectively. This improved activity and durability of the Pt{sub 2}In{sub 3} nanoparticles can make the catalyst an ideal catalyst candidate for direct alcohol fuel cell. - Graphical abstract: The ordered structure of Pt{sub 2}In{sub 3} nanoparticles synthesized by solvothermal method has confirmed through XRD and TEM. Cyclic voltametry and chronoamperometry showed improved catalytic activity and stability compared to commercial Pt/C. - Highlights: • Ordered Pt{sub 2}In{sub 3} nanoparticles were synthesized by solvothermal method. • Electrooxidation of alcohols on Pt{sub 2}In{sub 3} catalyst was investigated in acidic medium. • Pt{sub 2}In{sub 3} catalyst has superior catalytic activity compared to commercial Pt/C. • Pt{sub 2}In{sub 3} catalyst exhibited much higher stability than commercial Pt/C.

  12. Catalytic wet oxidation of phenol in a trickle bed reactor over a Pt/TiO2 catalyst.

    Science.gov (United States)

    Maugans, Clayton B; Akgerman, Aydin

    2003-01-01

    Catalytic wet oxidation of phenol was studied in a batch and a trickle bed reactor using 4.45% Pt/TiO2 catalyst in the temperature range 150-205 degrees C. Kinetic data were obtained from batch reactor studies and used to model the reaction kinetics for phenol disappearance and for total organic carbon disappearance. Trickle bed experiments were then performed to generate data from a heterogeneous flow reactor. Catalyst deactivation was observed in the trickle bed reactor, although the exact cause was not determined. Deactivation was observed to linearly increase with the cumulative amount of phenol that had passed over the catalyst bed. Trickle bed reactor modeling was performed using a three-phase heterogeneous model. Model parameters were determined from literature correlations, batch derived kinetic data, and trickle bed derived catalyst deactivation data. The model equations were solved using orthogonal collocations on finite elements. Trickle bed performance was successfully predicted using the batch derived kinetic model and the three-phase reactor model. Thus, using the kinetics determined from limited data in the batch mode, it is possible to predict continuous flow multiphase reactor performance.

  13. Single Pt Atoms Confined into a Metal-Organic Framework for Efficient Photocatalysis.

    Science.gov (United States)

    Fang, Xinzuo; Shang, Qichao; Wang, Yu; Jiao, Long; Yao, Tao; Li, Yafei; Zhang, Qun; Luo, Yi; Jiang, Hai-Long

    2018-02-01

    It is highly desirable yet remains challenging to improve the dispersion and usage of noble metal cocatalysts, beneficial to charge transfer in photocatalysis. Herein, for the first time, single Pt atoms are successfully confined into a metal-organic framework (MOF), in which electrons transfer from the MOF photosensitizer to the Pt acceptor for hydrogen production by water splitting under visible-light irradiation. Remarkably, the single Pt atoms exhibit a superb activity, giving a turnover frequency of 35 h -1 , ≈30 times that of Pt nanoparticles stabilized by the same MOF. Ultrafast transient absorption spectroscopy further unveils that the single Pt atoms confined into the MOF provide highly efficient electron transfer channels and density functional theory calculations indicate that the introduction of single Pt atoms into the MOF improves the hydrogen binding energy, thus greatly boosting the photocatalytic H 2 production activity. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. A facile template approach for the synthesis of mesoporous Fe3C/Fe-N-doped carbon catalysts for efficient and durable oxygen reduction reaction

    Institute of Scientific and Technical Information of China (English)

    Shuai Li; Bo Li; Liang Ma; Jia Yang; Hangxun Xu

    2017-01-01

    Facile synthetic approaches toward the development of efficient and durable nonprecious metal catalysts for the oxygen reduction reaction (ORR) are very important for commercializing advanced electrochemical devices such as fuel cells and metal-air batteries.Here we report a novel template approach to synthesize mesoporous Fe-N-doped carbon catalysts encapsulated with Fe3C nanoparticles.In this approach,the layer-structured FeOCl was first used as a template for the synthesis of a three-dimensional polypyrrole (PPy) structure.During the removal of the FeOCl template,the Fe3+ can be absorbed by PPy and then converted into Fe3C nanoparticles and Fe-N-C sites during the pyrolyzing process.As a result,the as-prepared catalysts could exhibit superior electrocatalytic ORR performance to the commercial Pt/C catalyst in alkaline solutions.Furthermore,the Zn-air battery assembled using the mesoporous carbon catalyst as the air electrode could surpass the commercial Pt/C catalyst in terms of the power density and energy density.

  15. Hydrogenation and hydrodeoxygenation of difurfurylidene acetone to liquid alkanes over Raney Ni and the supported Pt catalysts

    International Nuclear Information System (INIS)

    Li, Yuping; Huang, Xiaoming; Zhang, Qian; Chen, Lungang; Zhang, Xinghua; Wang, Tiejun; Ma, Longlong

    2015-01-01

    Highlights: • The C_8−C_1_4 alkane yield of 82.9% was obtained in the two-step hydrogenation/HDO process. • Protonation effect from methanol solvent increased F_2A conversion in the two-step process. • The rate-determining step was acyl C=O bond hydrogenation in the first step of F_2A hydrogenation. • The acidic centers from SiO_2−ZrO_2 activated the acyl and oxygen atoms of intermediates. • Acidity of SiO_2−ZrO_2 and Pt active centers of 1 wt%Pt/SiO_2−ZrO_2 resulted stable HDO performance. - Abstract: Direct HDO process for difurfurylidene acetone dimer (F_2A) conversion to liquid alkanes (C_8−C_1_4) at 260 °C in a batch reactor was investigated over different material supported 1 wt%Pt catalysts, including SAPO-11, HZSM-5, SiO_2−Al_2O_3, MCM-22, and home-made SiO_2−ZrO_2. C_8−C_1_4 alkanes of 55.8% was obtained over the optimized 1 wt%Pt/SiO_2−ZrO_2 due to its proper pore size of 9.0 nm and moderate acidic centers, together with more than 10% carbon yield of the oxygenated hydrocarbons, including C_1_1−C_1_3 chain alcohols & ketones and the hydrogenated F_2A dimers with furan ring (H-F_2A dimers). To improve the liquid alkane yield, a two-step process for F_2A conversion was also investigated, which included low-temperature hydrogenation at 50 °C over Raney Ni catalyst in a batch reactor and the subsequent high-temperature hydrodeoxygenation (HDO) at 280 °C over 1 wt%Pt/SiO_2−ZrO_2 in a fixed-bed reactor. The selectivity of 1,5-di(tetrahydro-2-furanyl)-3-pentanol (II-c) was the highest of 83.0% among the hydrogenated intermediates of H-F_2A dimers due to the protonation effect of methanol as the solvent and the hydrogenation of C=C bonds by Ni active centers. In the same time, the high content of this saturated alcohol H-dimer of II-C increased the solubility and stability of the intermediates in methanol solvent. High carbon yield of C_8−C_1_4 alkanes of 82.9%(mol) was obtained after oxygen atom removal from H-F_2A dimers via

  16. Efficient electrocatalytic performance of thermally exfoliated reduced graphene oxide-Pt hybrid

    Energy Technology Data Exchange (ETDEWEB)

    Antony, Rajini P., E-mail: raji.anna@gmail.com; Preethi, L.K.; Gupta, Bhavana; Mathews, Tom, E-mail: tom@igcar.gov.in; Dash, S.; Tyagi, A.K.

    2015-10-15

    Highlights: • Synthesis of Pt–RGO nanohybrids of very high electrochemically active surface area. • Electrocatalytic activity-cum-stability: ∼10 times that of commercial Pt-C catalyst. • TEM confirms narrow size distribution and excellent dispersion of Pt nanoparticles. • SAED and XRD indicate (1 1 1) orientation of Pt nanoparticles. • Methanol oxidation EIS reveal decrease in charge transfer resistance with potential - Abstract: High quality thermally exfoliated reduced graphene oxide (RGO) nanosheets decorated with platinum nanocrystals have been synthesized using a simple environmentally benign process. The electrocatalytic behaviour of the Pt–RGO nanohybrid for methanol oxidation was studied using cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy. High resolution transmission electron microscopy shows uniform dispersion of Pt nanoparticles of ∼2–4 nm size. X-ray diffraction and selected area diffraction studies reveal (1 1 1) orientation of the platinum nanoparticles. The cyclic voltammetry and chronoamperometry results indicate higher catalytic activity and stability for Pt–RGO compared to commercial Pt-C. The electrochemical active surface area of Pt–RGO (52.16 m{sup 2}/g) is found to be 1.5 times that of commercial Pt-C. Impedance spectroscopy shows different impedance behaviour at different potential regions, indicating change in methanol oxidation reaction mechanism with potential. The reversal of impedance pattern to the second quadrant, at potentials higher than ∼0.40 V, indicates change in the rate determining reaction.

  17. Green and efficient sample preparation method for the determination of catalyst residues in margarine by ICP-MS.

    Science.gov (United States)

    Hartwig, Carla Andrade; Pereira, Rodrigo Mendes; Novo, Diogo La Rosa; Oliveira, Dirce Taina Teixeira; Mesko, Marcia Foster

    2017-11-01

    Responding to the need for green and efficient methods to determine catalyst residues with suitable precision and accuracy in samples with high fat content, the present work evaluates a microwave-assisted ultraviolet digestion (MW-UV) system for margarines and subsequent determination of Ni, Pd and Pt using inductively coupled plasma mass spectrometry (ICP-MS). It was possible to digest up to 500mg of margarine using only 10mL of 4molL -1 HNO 3 with a digestion efficiency higher than 98%. This allowed the determination of catalyst residues using the ICP-MS and free of interferences. For this purpose, the following experimental parameters were evaluated: concentration of digestion solution, sample mass and microwave irradiation program. The residual carbon content was used as a parameter to evaluate the efficiency of digestion and to select the most suitable experimental conditions. The accuracy evaluation was performed by recovery tests using a standard solution and certified reference material, and recoveries ranging from 94% to 99% were obtained for all analytes. The limits of detection for Ni, Pd and Pt using the proposed method were 35.6, 0.264 and 0.302ngg -1 , respectively. When compared to microwave-assisted digestion (MW-AD) in closed vessels using concentrated HNO 3 (used as a reference method for sample digestion), the proposed MW-UV could be considered an excellent alternative for the digestion of margarine, as this method requires only a diluted nitric acid solution for efficient digestion. In addition, MW-UV provides appropriate solutions for further ICP-MS determination with suitable precision (relative standard deviation < 7%) and accuracy for all evaluated analytes. The proposed method was applied to margarines from different brands produced in Brazil, and the concentration of catalyst residues was in agreement with the current legislation or recommendations. Copyright © 2017 Elsevier B.V. All rights reserved.

  18. Theoretical evidence of PtSn alloy efficiency for CO oxidation.

    Science.gov (United States)

    Dupont, Céline; Jugnet, Yvette; Loffreda, David

    2006-07-19

    The efficiency of PtSn alloy surfaces toward CO oxidation is demonstrated from first-principles theory. Oxidation kinetics based on atomistic density-functional theory calculations shows that the Pt3Sn surface alloy exhibits a promising catalytic activity for fuel cells. At room temperature, the corresponding rate outstrips the activity of Pt(111) by several orders of magnitude. According to the oxidation pathways, the activation barriers are actually lower on Pt3Sn(111) and Pt3Sn/Pt(111) surfaces than on Pt(111). A generalization of Hammer's model is proposed to elucidate the key role of tin on the lowering of the barriers. Among the energy contributions, a correlation is evidenced between the decrease of the barrier and the strengthening of the attractive interaction energy between CO and O moieties. The presence of tin modifies also the symmetry of the transition states which are composed of a CO adsorbate on a Pt near-top position and an atomic O adsorption on an asymmetric mixed PtSn bridge site. Along the reaction pathways, a CO2 chemisorbed surface intermediate is obtained on all the surfaces. These results are supported by a thorough vibrational analysis including the coupling with the surface phonons which reveals the existence of a stretching frequency between the metal substrate and the CO2 molecule.

  19. Effect of TiO_2 Loading on Pt-Ru Catalysts During Alcohol Electrooxidation

    International Nuclear Information System (INIS)

    Hasa, Bjorn; Kalamaras, Evangelos; Papaioannou, Evangelos I.; Vakros, John; Sygellou, Labrini; Katsaounis, Alexandros

    2015-01-01

    Highlights: • TiO_2 can be used to modify Pt-Ru based electrodes for alcohol oxidation. • TiO_2 modified electrodes with lower amount of metals had higher active surface area than pure Pt-Ru electrodes. • TiO_2 modified electrodes showed comparable performance with pure Pt-Ru electrode both in a single cell and in a PEM fuel cell under alcohol fuelling. - Abstract: In this study, Pt-Ru based electrodes modified by TiO_2 were prepared by means of thermal decomposition of chloride and isopropoxide precursors on Ti substrates, characterised by X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), X-ray Photoelectron Spectroscopy (XPS), electrochemical techniques and CO stripping and used as anodes for alcohol oxidation. The minimization of the metal loading without electrocatalytic activity losses was also explored. TiO_2 was chosen due to its chemical stability, low cost and excellent properties as substrate for metal dispersion. It was found that TiO_2 loading up to 50% results in a 3-fold increase of the Electrochemically Active Surface (EAS). This conclusion has been confirmed by CO stripping experiments. All samples have been evaluated during the electrochemical oxidation of methanol, ethanol and glycerol. In all cases, the Pt_2_5-Ru_2_5-(TiO_2)_5_0 electrode had better electrocatalytic activity than the pure Pt_5_0-Ru_5_0 anode. The best modified electrode, (Pt_2_5-Ru_2_5-(TiO_2)_5_0), was also evaluated as anode in a PEM fuel cell under methanol fuelling conditions. The observed higher performance of the TiO_2 modified electrodes was attributed to the enhanced Pt-Ru dispersion as well as the formation of smaller Pt and Ru particles.

  20. Evaluation of Pt/C catalyst degradation and H2O2 formation changes under simulated PEM fuel cell condition by a rotating ring-disk electrode

    International Nuclear Information System (INIS)

    Ono, Kenshiro; Yasuda, Yuki; Sekizawa, Koshi; Takeuchi, Norimitsu; Yoshida, Toshihiko; Sudoh, Masao

    2013-01-01

    Potential cycling tests using 42.2 wt% and 19.1 wt% Pt/C catalysts were conducted by the RRDE technique to evaluate the changes in the electrochemical surface area (ECSA) and H 2 O 2 formation ability of the catalysts. As the typical operating conditions of a proton exchange membrane fuel cell (PEMFC), square wave potential cycling (0.7–0.9 V) was applied to the catalysts for 150,000 cycles in an O 2 -saturated 0.1 M HClO 4 electrolyte. During the potential cycling test, electrochemical measurements were carried out to characterize the ECSA, oxygen reduction reaction (ORR) activity and H 2 O 2 formation. After 150,000 potential cyclings, while the ECSA of the 42.2 wt% Pt/C dropped by 35%, the ECSA loss for the 19.1 wt% Pt/C was 55%. This result implies that the Pt content in the cathode catalyst affects the ECSA loss during the long-term PEMFC operation. Additionally, the H 2 O 2 formation ratio obviously increased with the potential cycling only in the case of the 19.1 wt% Pt/C. In order to verify the H 2 O 2 formation dependence on the ECSA, four types of catalysts, which included different Pt loading amounts (42.2, 28.1, 19.1 and 9.5 wt% Pt/C), were evaluated, and these results explained the relationship between the ECSA decay and H 2 O 2 formation increase in the durability tests

  1. Rapid in situ synthesis of spherical microflower Pt/C catalyst via spray-drying for high performance fuel cell application

    Energy Technology Data Exchange (ETDEWEB)

    Balgis, R.; Ogi, T.; Okuyama, K. [Department of Chemical Engineering, Graduate School of Engineering, Hiroshima University, Higashi Hiroshima, Hiroshima (Japan); Anilkumar, G.M.; Sago, S. [Research and Development Centre, Noritake Co., Ltd., Higashiyama, Miyoshi, Aichi (Japan)

    2012-08-15

    A facile route for the rapid in situ synthesis of platinum nanoparticles on spherical microflower carbon has been developed. An aqueous precursor slurry containing carbon black, polystyrene latex (PSL), polyvinyl alcohol, and platinum salt was spray-dried, followed by calcination to simultaneously reduce platinum salt and to decompose PSL particles. Prepared Pt/C catalyst showed high-performance electrocatalytic activity with excellent durability. The mass activity and specific activity values were 132.26 mA mg{sup -1} Pt and 207.62 {mu}A cm{sup -2} Pt, respectively. This work presents a future direction for the production of high-performance Pt/C catalyst in an industrial scale. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  2. Promotion of catalytic performance by adding W into Pt/ZrO{sub 2} catalyst for selective catalytic oxidation of ammonia

    Energy Technology Data Exchange (ETDEWEB)

    Sun, Mengmeng [Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu 610064, Sichuan (China); Wang, Suning; Li, Yuanshan [College of Chemical Engineering, Sichuan University, Chengdu 610064, Sichuan (China); Xu, Haidi, E-mail: xuhaidi@scu.edu.cn [Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu 610064, Sichuan (China); Chen, Yaoqiang, E-mail: nic7501@scu.edu.cn [Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu 610064, Sichuan (China); College of Chemical Engineering, Sichuan University, Chengdu 610064, Sichuan (China)

    2017-04-30

    Highlights: • The tungsten species weaken platinum-oxygen bond strength. • Pt{sup 0} was the active species of ammonia oxidation reaction in the low temperature. • Some PtO species could convert to Pt [111] beside WO{sub 3} species. - Abstract: Pt-WO{sub 3}/ZrO{sub 2} catalyst was prepared by co-impregnation method to improve the ammonia oxidation performance of Pt/ZrO{sub 2}. Differences in textural, structural, surface chemical states, redox properties and acid properties, together with the catalytic performance of Pt/ZrO{sub 2} and Pt-WO{sub 3}/ZrO{sub 2} catalysts were investigated systematically. The results of H{sub 2}-TPR revealed that higher reduction ability was possessed by Pt-WO{sub 3}/ZrO{sub 2} than that of Pt/ZrO{sub 2} due to the influence of tungsten on platinum. The XPS results showed that electron transfer from tungsten to platinum species made higher electron density around platinum. The TEM results revealed that the active lattice plane Pt[111] was obtained by modification of W species. Consequently, Pt-WO{sub 3}/ZrO{sub 2} exhibited obviously better ammonia oxidation performance compared with Pt/ZrO{sub 2}, the light-off temperature of NH{sub 3} shifted from 284 °C to 249 °C, the activation energy decreased from 113.4 kJ mol{sup −1} to 96.2 kJ mol{sup −1}.

  3. Electrocatalytic oxidation of methanol: study with Pt:Mo dispersed catalysts

    Directory of Open Access Journals (Sweden)

    Oliveira Neto Almir

    2000-01-01

    Full Text Available The electrocatalytic oxidation of methanol on Pt:Mo dispersed on carbon prepared using an alternative method recently developed in this laboratory was investigated. The EDX analysis confirmed that the simultaneous reduction of the precursor salts of Pt and Mo leads to the presence of these materials at the nominal composition initially calculated. The addition of Mo to Pt causes an increase of the oxidation currents, but does not improve the catalytic effect for methanol oxidation. Tafel plots for various methanol concentrations showed the presence of two slopes. On line differential electrochemical mass spectrometry (DEMS was used to investigate the distribution of products and intermediates in methanol oxidation.

  4. Selective catalytic reduction of NO{sub x} in lean-burn engine exhaust over a Pt/V/MCM-41 catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Jeon, Jong Yeol; Kim, Hee Young [Division of Advanced Chemical Technology, Korea Reasearch Institute of Chemical Technology, P.O. Box 107, Yusong, Taejon 305-600 (Korea, Republic of); Woo, Seong Ihl [Department of Chemical and Biomolecular Engineering, Center for Ultramicrochemical Process Systems, Korea Advanced Institute of Science and Technology, 373-1, Kusong-dong, Yusong-gu, Taejon, 305-701 (Korea, Republic of)

    2003-09-08

    The activities of Pt supported on various metal-substituted MCM-41 (V-, Ti-, Fe-, Al-, Ga-, La-, Co-, Mo-, Ce-, and Zr-MCM-41) and V-impregnated MCM-41 were investigated for the reduction of NO by C{sub 3}H{sub 6}. Among these catalysts, Pt supported on V-impregnated MCM-41 showed the best activity. The maximum conversion of NO into N{sub 2}+N{sub 2}O over this Pt/V/MCM-41 catalyst (Pt=1wt.%, V=3.8wt.%) was 73%, and this maximum conversion was sustained over a temperature range of 70C from 270 to 340C. The high activity of Pt/V/MCM-41 over a broad temperature range resulted from two additional reactions besides the reaction occurring on usual supported Pt, the reaction of NO with surface carbonaceous materials, and the reaction of NO occurring on support V-impregnated MCM-41. The former additional reaction showed an oscillation characteristic, a phenomenon in which the concentrations of parts of reactant and product gases oscillate continuously. At low temperature, some water vapor injected into the reactant gas mixture promoted the reaction occurring on usual supported Pt, whereas at high temperature, it suppressed the additional reaction related to carbonaceous materials. Five-hundred parts per million of SO{sub 2} added to the reactant gas mixture only slightly decreased the NO conversion of Pt/V/MCM-41.

  5. High-pressure vapor-phase hydrodeoxygenation of lignin-derived oxygenates to hydrocarbons by a PtMo bimetallic catalyst: Product selectivity, reaction pathway, and structural characterization

    Energy Technology Data Exchange (ETDEWEB)

    Yohe, Sara L.; Choudhari, Harshavardhan J.; Mehta, Dhairya D.; Dietrich, Paul J.; Detwiler, Michael D.; Akatay, Cem M.; Stach, Eric A.; Miller, Jeffrey T.; Delgass, W. Nicholas; Agrawal, Rakesh; Ribeiro, Fabio H.

    2016-12-01

    High-pressure, vapor-phase, hydrodeoxygenation (HDO) reactions of dihydroeugenol (2-methoxy-4-propylphenol), as well as other phenolic, lignin-derived compounds, were investigated over a bimetallic platinum and molybdenum catalyst supported on multi-walled carbon nanotubes (5%Pt2.5%Mo/MWCNT). Hydrocarbons were obtained in 100% yield from dihydroeugenol, including 98% yield of the hydrocarbon propylcyclohexane. The final hydrocarbon distribution was shown to be a strong function of hydrogen partial pressure. Kinetic analysis showed three main dihydroeugenol reaction pathways: HDO, hydrogenation, and alkylation. The major pathway occurred via Pt catalyzed hydrogenation of the aromatic ring and methoxy group cleavage to form 4-propylcyclohexanol, then Mo catalyzed removal of the hydroxyl group by dehydration to form propylcyclohexene, followed by hydrogenation of propylcyclohexene on either the Pt or Mo to form the propylcyclohexane. Transalkylation by the methoxy group occurred as a minor side reaction. Catalyst characterization techniques including chemisorption, scanning transmission electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy were employed to characterize the catalyst structure. Catalyst components identified were Pt particles, bimetallic PtMo particles, a Mo carbide-like phase, and Mo oxide phases.

  6. Influence of Sn content on PtSn/C catalysts for electrooxidation of C{sub 1}-C{sub 3} alcohols: Synthesis, characterization, and electrocatalytic activity

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jae Hong; Choi, Sung Mook; Nam, Sang Hoon; Seo, Min Ho; Kim, Won Bae [Department of Materials Science and Engineering, Gwangju Institute of Science and Technology (GIST), 261 Cheomdan-gwagiro, Buk-gu, Gwangju 500-712 (Korea); Choi, Sun Hee [Pohang Accelerator Laboratory, San-31 Hyoja-dong, Pohang, Kyungbuk 790-984 (Korea)

    2008-07-16

    A series of carbon-supported bimetallic PtSn catalysts for the electrooxidation of C{sub 1}-C{sub 3} alcohols (i.e., methanol (C{sub 1}), ethanol (C{sub 2}), and 1-propanol (C{sub 3})) were prepared with different Pt:Sn atomic ratios using borohydride reduction method combined with freeze-drying procedure at room temperature. The catalysts were investigated by employing various physicochemical analyses: X-ray diffraction (XRD), transmission electron microscopy (TEM) and extended X-ray absorption fine structure (EXAFS) to investigate the structural modification, and X-ray photoelectron spectroscopy (XPS) and X-ray absorption-near-edge spectroscopy (XANES) to characterize the change in electronic features. The variation of Sn content by forming PtSn alloys causes significant structural and electronic modifications of Pt crystallites, resulting in increases of lattice parameter and decreases of the Pt 5d band vacancies with Sn content. Cyclic voltammetry (CV) measurements showed that the addition of Sn into the Pt catalyst promotes the electro-catalytic activities for the electrooxidations of C{sub 1}, C{sub 2}, and C{sub 3} alcohols, in which the maximum activities appeared at different Sn contents for the C{sub 1}-C{sub 3} alcohols. In particular, a shift in optimum Pt:Sn composition was observed in that the Sn content required to reach the maximum peak current density was increased with the increasing number of carbon atoms in the C{sub 1}-C{sub 3} alcohols. Both the geometric and electronic effects with variation of Sn content are in close relationship in the bimetallic PtSn catalysts, consequently affecting the electrocatalytic activities by showing volcano-type behaviors over the electrooxidation of the individual alcohol. (author)

  7. Application of hydrophobic Pt catalysts in hydrogen isotopes separation from nuclear effluents

    Energy Technology Data Exchange (ETDEWEB)

    Ionita, G.; Popescu, I.; Stefanescu, I.; Retegan, T. [National Institute of Cryogenics and Isotopic Separation (Romania)

    2003-09-01

    According to reviewed references and to tests effected by authors the platinum/carbon/teflon is the most active and the most stable catalyst for removal of tritium from nuclear effluents by isotopic exchange between hydrogen and liquid water. To improve the performances of process it is recommended to use the catalyst as ordered or random mixed catalytic packing in a trickle bed reactor. (O.M.)

  8. Biobutanol as Fuel for Direct Alcohol Fuel Cells-Investigation of Sn-Modified Pt Catalyst for Butanol Electro-oxidation.

    Science.gov (United States)

    Puthiyapura, Vinod Kumar; Brett, Dan J L; Russell, Andrea E; Lin, Wen-Feng; Hardacre, Christopher

    2016-05-25

    Direct alcohol fuel cells (DAFCs) mostly use low molecular weight alcohols such as methanol and ethanol as fuels. However, short-chain alcohol molecules have a relative high membrane crossover rate in DAFCs and a low energy density. Long chain alcohols such as butanol have a higher energy density, as well as a lower membrane crossover rate compared to methanol and ethanol. Although a significant number of studies have been dedicated to low molecular weight alcohols in DAFCs, very few studies are available for longer chain alcohols such as butanol. A significant development in the production of biobutanol and its proposed application as an alternative fuel to gasoline in the past decade makes butanol an interesting candidate fuel for fuel cells. Different butanol isomers were compared in this study on various Pt and PtSn bimetallic catalysts for their electro-oxidation activities in acidic media. Clear distinctive behaviors were observed for each of the different butanol isomers using cyclic voltammetry (CV), indicating a difference in activity and the mechanism of oxidation. The voltammograms of both n-butanol and iso-butanol showed similar characteristic features, indicating a similar reaction mechanism, whereas 2-butanol showed completely different features; for example, it did not show any indication of poisoning. Ter-butanol was found to be inactive for oxidation on Pt. In situ FTIR and CV analysis showed that OHads was essential for the oxidation of primary butanol isomers which only forms at high potentials on Pt. In order to enhance the water oxidation and produce OHads at lower potentials, Pt was modified by the oxophilic metal Sn and the bimetallic PtSn was studied for the oxidation of butanol isomers. A significant enhancement in the oxidation of the 1° butanol isomers was observed on addition of Sn to the Pt, resulting in an oxidation peak at a potential ∼520 mV lower than that found on pure Pt. The higher activity of PtSn was attributed to the

  9. Thermal desorption (TD) study of heterogeneous catalytic reactions--4. Nonuniformity of Pt/. gamma. -Al/sub 2/O/sub 3/ catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Rozanov, V V [Inst. Chem. Phys. Acad. Sci. U.S.S.R.; Sklyarov, A V; Gland, J

    1979-10-01

    Programed TD of n-heptane adsorbed on 0.6-3% by wt Pt/..gamma..-Al/sub 2/O/sub 3/ laboratory catalysts with different dispersities of the metallic phase showed the formation of toluene at 160/sup 0/-260/sup 0/C with spectral maxima at about 200/sup 0/ and 230/sup 0/C and a benzene desorption maxima at 300/sup 0/C. The desorption of both benzene and the high-temperature form of toluene decreased with decreased dispersity of the catalyst and was not observed with the catalyst characterized by an average Pt particle size of 1000 A. Toluene adsorbed on the same catalysts showed a TD peak of benzene at 300/sup 0/C. With commercial Pt/Al/sub 2/O/sub 3/ reforming catalysts, up to five toluene desorption peaks were observed at 200/sup 0/-360/sup 0/C, suggesting the presence of active sites with different activities and concentrations on the catalyst surface. Experiments on TD of deuterated n-heptane suggested different reaction mechanisms associated with different types of active sites and the formation of low- and high-temperature forms of toluene. Only the latter had a maximum coinciding with a TD peak of D/sub 2/ (240/sup 0/C), probably formed by dehydrogenation of adsorbed diene or olefin intermediates.

  10. 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...

  11. Atomic layer deposition synthesis and evaluation of core–shell Pt-WC electrocatalysts

    International Nuclear Information System (INIS)

    Hsu, Irene J.; Chen, Jingguang G.; Jiang, Xiaoqiang; Willis, Brian G.

    2015-01-01

    Pt-WC core shell particles were produced using atomic layer deposition (ALD) to deposit Pt layers onto WC particle substrates. A range of Pt depositions were used to determine the growth mechanism for the Pt-WC powder system. TEM imaging and Cu stripping voltammetry found that Pt ALD growth on WC powder substrates was similar to that on WC thin films. However, excess free carbon was found to affect Pt ALD by blocking adsorption sites on WC. The Pt-WC samples were evaluated for the oxygen reduction reaction using a rotating disk electrode to obtain quantitative activity information. The mass and specific activities for the 30 and 50 ALD cycle samples were found to be comparable to a 10 wt. % Pt/C catalyst. However, higher overpotentials and lower limiting currents were observed with ALD Pt-WC compared to Pt/C catalysts, indicating that the oxygen reduction mechanism is not as efficient on Pt-WC as on bulk Pt. Additionally, these Pt-WC catalysts were used to demonstrate hydrogen evolution reaction activity and were found to perform as well as bulk Pt catalyst but with a fraction of the Pt loading, in agreement with the previous work on Pt-WC thin film catalysts

  12. bis-Nitrile and bis-Dialkylcyanamide Platinum(II) Complexes as Efficient Catalysts for Hydrosilylation Cross-Linking of Siloxane Polymers.

    Science.gov (United States)

    Islamova, Regina M; Dobrynin, Mikhail V; Ivanov, Daniil M; Vlasov, Andrey V; Kaganova, Elena V; Grigoryan, Galina V; Kukushkin, Vadim Yu

    2016-03-05

    cis- and trans-Isomers of the platinum(II) nitrile complexes [PtCl2(NCR)2] (R = NMe2, N(C₅H10), Ph, CH2Ph) were examined as catalysts for hydrosilylation cross-linking of vinyl-terminated polydimethylsiloxane and trimethylsilyl-terminated poly(dimethylsiloxane-co-ethylhydrosiloxane) producing high quality silicone rubbers. Among the tested platinum species the cis-complexes are much more active catalysts than their trans-congeners and for all studied platinum complexes cis-[PtCl2(NCCH2Ph)2] exhibits the best catalytic activity (room temperature, c = 1.0 × 10(-4) mol/L, τpot-life 60 min, τcuring 6 h). Although cis-[PtCl₂(NCCH2Ph)2] is less active than the widely used Karstedt's catalyst, its application for the cross-linking can be performed not only at room temperature (c = 1.0 × 10(-4) mol/L), but also, more efficiently, at 80 °C (c = 1.0 × 10(-4)-1.0 × 10(-5) mol/L) and it prevents adherence of the formed silicone rubbers to equipment. The usage of the cis- and trans-[PtCl2(NCR)2] complexes as the hydrosilylation catalysts do not require any inhibitors and, moreover, the complexes and their mixtures with vinyl- and trimethylsilyl terminated polysiloxanes are shelf-stable in air. Tested catalysts do not form colloid platinum particles after the cross-linking.

  13. Pd-Pt alloys nanowires as support-less electrocatalyst with high synergistic enhancement in efficiency for methanol oxidation in acidic medium.

    Science.gov (United States)

    Rana, Moumita; Patil, Pramod K; Chhetri, Manjeet; Dileep, K; Datta, Ranjan; Gautam, Ujjal K

    2016-02-01

    In a facile approach, Pd73Pt27 alloy nanowires (NWs) with large aspect ratios were synthesized in high yield by using sacrificial templates. Unlike majority of processes, our synthesis was carried out in aqueous solution with no intermittent separating stages for the products, while maintaining the NW morphology up to ∼30% of Pt. Upon evaporation of their dispersion, the NWs transform into a stable porous membrane due to self-entanglement and can be directly lifted and employed for electrocatalytic applications without external catalyst supports. We show that the NW membranes exhibit efficient electrocatalytic performance for methanol oxidation reaction (MOR) with 10 times higher mass activity and 4.4 times higher specific activity in acidic media as compared to commercial Pt catalysts. The membrane electrocatalysts is robust and exhibited very good stability with retention of ∼70% mass-activity after 4000 potential cycles. Since Pd was found to be inert towards MOR in acidic medium, our investigation provides a direct estimate of synergistic enhancement of efficiency. Over 10 times increment of mass activity appears to be significantly higher than previous investigations in various other reaction media. Copyright © 2015 Elsevier Inc. All rights reserved.

  14. Catalytic Hydrogenation and Hydrodeoxygenation of Furfural over Pt(111): A Model System for the Rational Design and Operation of Practical Biomass Conversion Catalysts

    OpenAIRE

    Taylor, Martin J.; Jiang, Li; Reichert, Joachim; Papageorgiou, Anthoula C.; Beaumont, Simon K.; Wilson, Karen; Lee, Adam F.; Barth, Johannes V.; Kyriakou, Georgios

    2017-01-01

    Furfural is a key bioderived platform chemical whose reactivity under hydrogen atmospheres affords diverse chemical intermediates. Here, temperature-programmed reaction spectrometry and complementary scanning tunneling microscopy (STM) are employed to investigate furfural adsorption and reactivity over a Pt(111) model catalyst. Furfural decarbonylation to furan is highly sensitive to reaction conditions, in particular, surface crowding and associated changes in the adsorption geometry: furfur...

  15. Acetylene and carbon monoxide oxidation over a Pt/Rh/CeO2/γ-Al2O3 automotive exhaust gas catalyst: kinetic modelling of transient experiments

    NARCIS (Netherlands)

    Harmsen, J.M.A.; Hoebink, J.H.B.J.; Schouten, J.C.

    2001-01-01

    The transient kinetics of acetylene (C2H2) conversion by oxygen over a commercial Pt/Rh/CeO2/¿-Al2O3 three-way catalyst have been modelled. Experiments to validate the model were carried out in a fixed-bed reactor with two separate inlets, enabling alternate feeding of acetylene and oxygen.

  16. Kinetic modeling of hydrocracking reaction in a trickle-bed reactor with Pt/Y-zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Lee, BalSang; Park, Myung-June; Kim, Young-A; Park, Eun Duck [Ajou University, Suwon (Korea, Republic of); Han, Jeongsik [Agency for Defense Development, Daejeon (Korea, Republic of); Jeong, Kwang-Eun; Kim, Chul-Ung; Jeong, Soon-Yong [Korea Research Institute of Chemical Technology (KRICT), Daejeon (Korea, Republic of)

    2014-03-15

    A kinetic model is developed to predict the entire distribution of hydrocarbon products for the hydrocracking reaction with Pt/Y-zeolite catalysts in a trickle-bed reactor. Operating conditions, such as temperature, pressure, and wax and H{sub 2} flow rates were varied to evaluate their effects on conversion and distribution, and kinetic parameters were estimated using the experimental data that covers the window of operating conditions. The comparison between experimental data and simulated results corroborated the validity of the developed model, and the quantitative prediction of the reactor performance was clearly demonstrated. To make evident the usefulness of the model, an optimization method, genetic algorithm (GA), was applied, and the optimal condition for the maximum production of C{sub 10}-C{sub 17} was successfully calculated.

  17. Kinetic modeling of hydrocracking reaction in a trickle-bed reactor with Pt/Y-zeolite catalysts

    International Nuclear Information System (INIS)

    Lee, BalSang; Park, Myung-June; Kim, Young-A; Park, Eun Duck; Han, Jeongsik; Jeong, Kwang-Eun; Kim, Chul-Ung; Jeong, Soon-Yong

    2014-01-01

    A kinetic model is developed to predict the entire distribution of hydrocarbon products for the hydrocracking reaction with Pt/Y-zeolite catalysts in a trickle-bed reactor. Operating conditions, such as temperature, pressure, and wax and H 2 flow rates were varied to evaluate their effects on conversion and distribution, and kinetic parameters were estimated using the experimental data that covers the window of operating conditions. The comparison between experimental data and simulated results corroborated the validity of the developed model, and the quantitative prediction of the reactor performance was clearly demonstrated. To make evident the usefulness of the model, an optimization method, genetic algorithm (GA), was applied, and the optimal condition for the maximum production of C 10 -C 17 was successfully calculated

  18. Sulfated polyborate: A mild, efficient catalyst for synthesis of N-tert ...

    Indian Academy of Sciences (India)

    Rapid, efficient and inexpensive method for synthesis of N-tert-butyl/N-trityl protected amides via Ritter reaction of nitriles with tertiary alcohols in the presence of a sulfated polyborate catalyst under solvent-free conditions is described. The catalyst has the advantage of Lewis as well as Bronsted acidity and recyclability ...

  19. Silica nanoparticles as a highly efficient catalyst for the one-pot ...

    African Journals Online (AJOL)

    Silica nanoparticles as a highly efficient catalyst for the one-pot synthesis of sterically congested ... Bulletin of the Chemical Society of Ethiopia ... 42 nm) as a catalyst under solvent free conditions at room temperature is described. The ease of ...

  20. Highly selective hydrogenation of furfural to furfuryl alcohol over Pt nanoparticles supported on g-C3N4 nanosheets catalysts in water

    Science.gov (United States)

    Chen, Xiufang; Zhang, Ligang; Zhang, Bo; Guo, Xingcui; Mu, Xindong

    2016-06-01

    Graphitic carbon nitride nanosheets were investigated for developing effective Pt catalyst supports for selective hydrogenation of furfural to furfuryl alcohol in water. The nanosheets with an average thickness of about 3 nm were synthesized by a simple and green method through thermal oxidation etching of bulk g-C3N4 in air. Combined with the unique feature of nitrogen richness and locally conjugated structure, the g-C3N4 nanosheets with a high surface area of 142 m2 g-1 were demonstrated to be an excellent supports for loading small-size Pt nanoparticles. Superior furfural hydrogenation activity in water with complete conversion of furfural and high selectivity of furfuryl alcohol (>99%) was observed for g-C3N4 nanosheets supported Pt catalysts. The large specific surface area, uniform dispersion of Pt nanoparticles and the stronger furfural adsorption ability of nanosheets contributed to the considerable catalytic performance. The reusability tests showed that the novel Pt catalyst could maintain high activity and stability in the furfural hydrogenation reaction.

  1. Highly selective hydrogenation of furfural to furfuryl alcohol over Pt nanoparticles supported on g-C3N4 nanosheets catalysts in water.

    Science.gov (United States)

    Chen, Xiufang; Zhang, Ligang; Zhang, Bo; Guo, Xingcui; Mu, Xindong

    2016-06-22

    Graphitic carbon nitride nanosheets were investigated for developing effective Pt catalyst supports for selective hydrogenation of furfural to furfuryl alcohol in water. The nanosheets with an average thickness of about 3 nm were synthesized by a simple and green method through thermal oxidation etching of bulk g-C3N4 in air. Combined with the unique feature of nitrogen richness and locally conjugated structure, the g-C3N4 nanosheets with a high surface area of 142 m(2) g(-1) were demonstrated to be an excellent supports for loading small-size Pt nanoparticles. Superior furfural hydrogenation activity in water with complete conversion of furfural and high selectivity of furfuryl alcohol (>99%) was observed for g-C3N4 nanosheets supported Pt catalysts. The large specific surface area, uniform dispersion of Pt nanoparticles and the stronger furfural adsorption ability of nanosheets contributed to the considerable catalytic performance. The reusability tests showed that the novel Pt catalyst could maintain high activity and stability in the furfural hydrogenation reaction.

  2. Dissolution kinetics of Pd and Pt from automobile catalysts by naturally occurring complexing agents

    Czech Academy of Sciences Publication Activity Database

    Šebek, O.; Mihaljevič, M.; Strnad, L.; Ettler, V.; Ježek, J.; Štědrý, R.; Drahota, P.; Ackerman, Lukáš; Adamec, V.

    2011-01-01

    Roč. 198, December (2011), s. 331-339 ISSN 0304-3894 Institutional research plan: CEZ:AV0Z30130516 Keywords : automobile catalyst * Platinum group elements * mobilisation * leaching * kinetic Subject RIV: DD - Geochemistry Impact factor: 4.173, year: 2011

  3. Catalytic reforming of glycerol in supercritical water over bimetallic Pt-Ni catalyst

    NARCIS (Netherlands)

    Chakinala, A.G.; van Swaaij, Willibrordus Petrus Maria; Kersten, Sascha R.A.; de Vlieger, Dennis; Seshan, Kulathuiyer; Brilman, Derk Willem Frederik

    2013-01-01

    Catalytic reforming of pure glycerol for the production of hydrogen at low temperature and short residence times in supercritical water was investigated using a bimetallic Pt–Ni catalyst supported on alumina. Initial tests were carried out to study the reforming activity of bimetallic Pt–Ni

  4. Hydrogen peroxide modified Mg-Al-O oxides supported Pt-Sn catalysts for paraffin dehydrogenation

    NARCIS (Netherlands)

    Lai, Y.; He, Songbo; Luo, S.; Bi, W.; Li, XianRu; Sun, Chenglin; Seshan, Kulathuiyer

    2015-01-01

    In this work, a new method to prepare Mg–Al–O oxide by co-precipitation method with addition of H2O2 was developed. The application of Mg–Al–O as a support of Pt–Sn catalysts for paraffin dehydrogenation was investigated. Characterization results indicated that modification of H2O2 (i) enlarged the

  5. Cu-exchanged heteropoly acids as efficient and reusable catalysts ...

    Indian Academy of Sciences (India)

    Administrator

    neous catalysts has received considerable interest in different areas of organic ... easily recovered from the reaction mixture by simple filtration and can be re-used after ..... Acknowledgements. We gratefully acknowledge the financial support.

  6. Efficient utilization of bimetallic catalyst in low environment syngas ...

    Indian Academy of Sciences (India)

    Sonal

    2017-10-26

    Oct 26, 2017 ... Department of Chemical Engineering, Indian Institute of Technology, ... MS received 27 May 2017; revised 21 August 2017; accepted 31 ... The catalysts were tested in fixed bed reactor at industrial relevant FTS conditions.

  7. 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.

  8. Size-dependent effects in supported highly dispersed Fe2O3 catalysts, doped with Pt and Pd

    International Nuclear Information System (INIS)

    Cherkezova-Zheleva, Zara; Shopska, Maya; Mitov, Ivan; Kadinov, Georgi

    2010-01-01

    Series of Fe and Fe–Me (Me = Pt or Pd) catalyst supported on γ-Al 2 O 3 , TiO 2 (anatase) or diatomite were prepared by the incipient wetness impregnation method. The metal loading was 8 wt.% Fe and 0.7 wt.% noble metal. The preparation and pretreatment conditions of all studied samples were kept to be the same. X-ray diffraction, Moessbauer spectroscopy, X-ray photoelectron spectroscopy and temperature-programmed reduction are used for characterization of the supports and the samples at different steps during their treatment and catalytic tests. The catalytic activity of the samples was tested in the reaction of total benzene oxidation. The physicochemical and catalytic properties of the obtained materials are compared with respect of the different chemical composition, dispersion of used carriers and of the supported phases. Samples with the same composition prepared by mechanical mixing are studied as catalysts for comparison and for clearing up the presence of size-dependent effect, also.

  9. Pt-Ru/CeO2/carbon nanotube nanocomposites: an efficient electrocatalyst for direct methanol fuel cells.

    Science.gov (United States)

    Sun, Zhenyu; Wang, Xiang; Liu, Zhimin; Zhang, Hongye; Yu, Ping; Mao, Lanqun

    2010-07-20

    Pt-Ru/CeO(2)/multiwalled carbon nanotube (MWNT) electrocatalysts were prepared using a rapid sonication-facilitated deposition method and were characterized by X-ray diffraction (XRD), X-ray photoemission spectroscopy (XPS), transmission electron microscopy (TEM), energy-dispersive spectroscopy (EDS), and voltammetry. Morphological characterization by TEM revealed that CeO(2) nanoparticles (NPs) were in intimate contact with Pt-Ru NPs, and both were highly dispersed on the exteriors of nanotubes with a small size and a very narrow size distribution. Compared with the Pt-Ru/MWNT and Pt/MWNT electrocatalysts, the as-prepared Pt-Ru/CeO(2)/MWNT exhibited a significantly improved electrochemically active surface area (ECSA) and a remarkably enhanced activity toward methanol oxidation. The effects of the Pt-Ru loading and the Pt-to-Ru molar ratio on the electrocatalytic activity of Pt-Ru/CeO(2)/MWNT for methanol oxidation were investigated. We found that a maximum activity toward methanol oxidation reached at the 10 wt % of Pt-Ru loading and 1:1 of Pt-to-Ru ratio. Moreover, the role of CeO(2) in the catalysts for the enhancement of methanol oxidation was discussed in terms of both bifunctional mechanism and electronic effects.

  10. 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.

  11. Boosting the performance of Pt electro-catalysts toward formic acid electro-oxidation by depositing sub-monolayer Au clusters

    International Nuclear Information System (INIS)

    Bi Xuanxuan; Wang Rongyue; Ding Yi

    2011-01-01

    Highlights: → Au decoration on Pt nanoparticles simultaneously increases the activity and stability. → Sub-monolayer Au decoration changes the reaction path and results in the activity improvement. → Increasing the Au coverage will increase the specific activity. → Proper Au coverage results in a maximum mass specific activity. - Abstract: CO poisoning is the main obstacle to the application of Pt nanoparticles as anode catalysts in direct formic acid fuel cells (DFAFCs). Significant types of Pt alloys have been investigated, which often demonstrate evidently improved catalytic performance governed by difference mechanisms. By using a well-known electrochemical technique of under potential deposition and in situ redox replacement, sub-monolayer Au clusters are deposited onto Pt nanoparticle surfaces in a highly controlled manner, generating a unique surface alloy structure. Under optimum conditions, the modified Pt nanoparticles can exhibit greatly enhanced specific activity (up to 23-fold increase) at potential of -0.2 V vs. MSE toward formic acid electro-oxidation (FAEO). Interestingly, the mass specific activity can also be improved by a factor of 2.3 at potential of -0.35 V vs. MSE although significant amount of surface Pt atoms are covered by the overlayer Au clusters. The much enhanced catalytic activity can be ascribed to a Pt surface ensemble effect, which induces change of the reaction path. Moreover, the sub-monolayer Au coating on the surface also contributes to the enhanced catalyst durability by inhibiting the Pt oxidation. These results show great potential to rationally design more active and stable nanocatalysts by modifying the Pt surface with otherwise inactive materials.

  12. Synthesis of Supported NiPt Bimetallic Nanoparticles, Methods for Controlling the Surface Coverage of Ni Nanoparticles With Pt, Methods Of Making NiPt Multilayer Core-Shell Structures and Application of the Supported Catalysts for CO2 Reforming

    KAUST Repository

    Li, Lidong; Anjum, Dalaver H.; Zhou, Lu; Laveille, Paco; Basset, Jean-Marie

    2015-01-01

    Embodiments of the present disclosure provide for supported Ni/Pt bimetallic nanoparticles, compositions including supported NiPt nanoparticles, methods of making supported NiPt nanoparticles, methods of using supported NiPt nanoparticles

  13. Synthesis of Supported NiPt Bimetallic Nanoparticles, Methods for Controlling the Surface Coverage of Ni Nanoparticles With Pt, Methods Of Making NiPt Multilayer Core-Shell Structures and Application of the Supported Catalysts for CO2 Reforming

    KAUST Repository

    Li, Lidong

    2015-06-25

    Embodiments of the present disclosure provide for supported Ni/Pt bimetallic nanoparticles, compositions including supported NiPt nanoparticles, methods of making supported NiPt nanoparticles, methods of using supported NiPt nanoparticles, and the like.

  14. Catalytic decomposition of trichloroethylene over Pt-/Ni-catalyst under microwave heating

    Energy Technology Data Exchange (ETDEWEB)

    Takashima, Hideaki; Karches, Martin [Chemiace Laboratory, 36-13 Hon-cho, Hachioji 192-0066 (Japan); Kanno, Yoshinori [Interdisciplinary Graduate School of Medicine and Engineering, University of Yamanashi, 4-3-11 Takeda, Kofu 400-8511 (Japan)], E-mail: kanno@yamanashi.ac.jp

    2008-01-30

    Microwave (MW)-activated catalytic reactor system was studied and the results were compared with that of a conventional system based on the thermal activation method. Trichloroethylene (TCE) was decomposed under various MW-powers supply. Results showed that there is an optimum film thickness that was loaded on supports in MW heating system. The threshold may be within 1-3 {mu}m. Lower temperature cannot activate the catalyst, while higher temperature results in carbon deposition and catalyst deactivation. This means that the dechlorination reaction needs to fix an optimum film MW-power supply in order to avoid the deposition of carbon on the surface of the active phase. MW-activated system is also worth compensating the conventional system in VOCs decomposition reaction.

  15. Polymeric carbon nitride/mesoporous silica composites as catalyst support for Au and Pt nanoparticles.

    Science.gov (United States)

    Xiao, Ping; Zhao, Yanxi; Wang, Tao; Zhan, Yingying; Wang, Huihu; Li, Jinlin; Thomas, Arne; Zhu, Junjiang

    2014-03-03

    Small and homogeneously dispersed Au and Pt nanoparticles (NPs) were prepared on polymeric carbon nitride (CNx )/mesoporous silica (SBA-15) composites, which were synthesized by thermal polycondensation of dicyandiamide-impregnated preformed SBA-15. By changing the condensation temperature, the degree of condensation and the loading of CNx can be controlled to give adjustable particle sizes of the Pt and Au NPs subsequently formed on the composites. In contrast to the pure SBA-15 support, coating of SBA-15 with polymeric CNx resulted in much smaller and better-dispersed metal NPs. Furthermore, under catalytic conditions the CNx coating helps to stabilize the metal NPs. However, metal NPs on CNx /SBA-15 can show very different catalytic behaviors in, for example, the CO oxidation reaction. Whereas the Pt NPs already show full CO conversion at 160 °C, the catalytic activity of Au NPs seems to be inhibited by the CNx support. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  16. Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media

    International Nuclear Information System (INIS)

    Stojmenović, Marija; Momčilović, Milan; Gavrilov, Nemanja; Pašti, Igor A.; Mentus, Slavko; Jokić, Bojan; Babić, Biljana

    2015-01-01

    Ordered mesoporous carbon, volume-doped up to 3 w.% with Pt, Ru and Pt-Ru nanoparticles was synthesized by evaporation-induced self-assembly method, under acidic conditions. The content of incorporated metal was determined by EDX analysis. The X-ray diffractometry confirmed the existence of highly dispersed metallic phases in doped samples. Specific surface area was determined by N 2 -physisorption measurements to range between 452 and 545 m 2 g −1 . Raman spectroscopy of investigated materials indicated highly disordered carbon structure with crystallite sizes around 1.4 nm. In a form of thin-layer electrode on glassy carbon support, in 0.1 M KOH solution, the prepared materials displayed high activity toward oxygen reduction reaction (ORR) in alkaline media, with onset potentials more positive than −0.10 V vs. SCE. The kinetics of O 2 reduction was found to be affected by both the specific surface area and the concentration of metal dopants. The ethanol tolerance of (Pt, Ru)-doped OMCs was found to be higher than that of common Pt/C ORR catalysts. Presented study provides a new route for the synthesis of active and selective ORR catalysts in alkaline media, being competitive with, or superior to, the existing ones in terms of performance and price

  17. Ethanol electrooxidation on a carbon-supported Pt catalyst at elevated temperature and pressure: A high-temperature/high-pressure DEMS study

    Science.gov (United States)

    Sun, S.; Halseid, M. Chojak; Heinen, M.; Jusys, Z.; Behm, R. J.

    The electrooxidation of ethanol on a Pt/Vulcan catalyst was investigated in model studies by on-line differential electrochemical mass spectrometry (DEMS) over a wide range of reaction temperatures (23-100 °C). Potentiodynamic and potentiostatic measurements of the Faradaic current and the CO 2 formation rate, performed at 3 bar overpressure under well-defined transport and diffusion conditions reveal significant effects of temperature, potential and ethanol concentration on the total reaction activity and on the selectivity for the pathway toward complete oxidation to CO 2. The latter pathway increasingly prevails at higher temperature, lower concentration and lower potentials (∼90% current efficiency for CO 2 formation at 100 °C, 0.01 M, 0.48 V), while at higher ethanol concentrations (0.1 M), higher potentials or lower temperatures the current efficiency for CO 2 formation drops, reaching values of a few percent at room temperature. These trends result in a significantly higher apparent activation barrier for complete oxidation to CO 2 (68 ± 2 kJ mol -1 at 0.48 V, 0.1 M) compared to that of the overall ethanol oxidation reaction determined from the Faradaic current (42 ± 2 kJ mol -1 at 0.48 V, 0.1 M). The mechanistic implications of these results and the importance of relevant reaction and mass transport conditions in model studies for reaction predictions in fuel cell applications are discussed.

  18. Controllable synthesis of Co3O4 nanocrystals as efficient catalysts for oxygen reduction reaction

    Science.gov (United States)

    Li, Baoying; Zhang, Yihe; Du, Ruifeng; Liu, Lei; Yu, Xuelian

    2018-03-01

    The electrochemical oxygen reduction reaction (ORR) has received great attention due to its importance in fuel cells and metal-air batteries. Here, we present a simple approach to prepare non-noble metal catalyst-Co3O4 nanocrystals (NCs). The particle size and shape were simply controlled by different types and concentrations of metal precursor. Furthermore, different sizes and shapes of Co3O4 NCs are explored as electrocatalysts for ORR, and it has been observed that particles with a similar shape, and smaller particle size led to greater catalytic current densities because of the greater surface area. For particles with a comparable size, the shape or crystalline structure governed the activity of the electrocatalytic reactions. Most importantly, the 9 nm-Co3O4 were demonstrated to act as low-cost catalysts for the ORR with a similar performance to that of Pt catalysts.

  19. Stability investigation of a high number density Pt1/Fe2O3 single-atom catalyst under different gas environments by HAADF-STEM

    Science.gov (United States)

    Duan, Sibin; Wang, Rongming; Liu, Jingyue

    2018-05-01

    Catalysis by supported single metal atoms has demonstrated tremendous potential for practical applications due to their unique catalytic properties. Unless they are strongly anchored to the support surfaces, supported single atoms, however, are thermodynamically unstable, which poses a major obstacle for broad applications of single-atom catalysts (SACs). In order to develop strategies to improve the stability of SACs, we need to understand the intrinsic nature of the sintering processes of supported single metal atoms, especially under various gas environments that are relevant to important catalytic reactions. We report on the synthesis of high number density Pt1/Fe2O3 SACs using a facial strong adsorption method and the study of the mobility of these supported Pt single atoms at 250 °C under various gas environments that are relevant to CO oxidation, water–gas shift, and hydrogenation reactions. Under the oxidative gas environment, Fe2O3 supported Pt single atoms are stable even at high temperatures. The presence of either CO or H2 molecules in the gas environment, however, facilitates the movement of the Pt atoms. The strong interaction between CO and Pt weakens the binding between the Pt atoms and the support, facilitating the movement of the Pt single atoms. The dissociation of H2 molecules on the Pt atoms and their subsequent interaction with the oxygen species of the support surfaces dislodge the surface oxygen anchored Pt atoms, resulting in the formation of Pt clusters. The addition of H2O molecules to the CO or H2 significantly accelerates the sintering of the Fe2O3 supported Pt single atoms. An anchoring-site determined sintering mechanism is further proposed, which is related to the metal–support interaction.

  20. Quaternary Pt{sub 2}Ru{sub 1}Fe{sub 1}M{sub 1}/C (M=Ni, Mo, or W) catalysts for methanol electro-oxidation reaction

    Energy Technology Data Exchange (ETDEWEB)

    Jeon, Min Ku; Lee, Ki Rak; Kang, Kweon Ho; Park, Geun Il [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of); Jeon, Hyung Joon [Kyoto University, Kyoto (Japan); McGinn, Paul J. [University of Notre Dame, Indiana (United States)

    2015-02-15

    Quaternary Pt{sub 2}Ru{sub 1}Fe{sub 1}M{sub 1}/C (M=Ni, Mo, or W) catalysts were investigated for the methanol electro-oxidation reaction (MOR). Electrocatalytic activities of the quaternary catalysts for CO electro-oxidation were studied via CO stripping experiments, and the Pt{sub 2}Ru{sub 1}Fe{sub 1}Ni{sub 1}/C and Pt{sub 2}Ru{sub 1}Fe{sub 1}W{sub 1}/C catalysts exhibited lowered on-set potential compared to that of a commercial PtRu/C catalyst. MOR activities of the quaternary catalysts were determined by linear sweep voltammetry (LSV) experiments, and the Pt{sub 2}Ru{sub 1}Fe{sub 1}W{sub 1}/C catalyst outperformed the commercial PtRu/C catalyst by 170 and 150% for the mass and specific activities, respectively. X-ray photoelectron spectroscopy (XPS) was employed to analyze surface oxidation states of constituent atoms, and it was identified that the structure of the synthesized catalysts are close to a nano-composite of Pt and constituent metal hydroxides and oxides. In addition, the XPS results suggested that the bi-functional mechanism accounts for the improved performance of the Pt{sub 2}Ru{sub 1}Fe{sub 1}Ni{sub 1}/C and Pt{sub 2}Ru{sub 1} Fe{sub 1}W{sub 1}/C catalysts.

  1. Understanding of the structure activity relationship of PtPd bimetallic catalysts prepared by surface organometallic chemistry and ion exchange during the reaction of iso-butane with hydrogen

    KAUST Repository

    Al-Shareef, Reem A.; Harb, Moussab; Saih, Youssef; Ould-Chikh, Samy; Roldan, Manuel A.; Anjum, Dalaver H.; Guyonnet, Elodie Bile; Candy, Jean-Pierre; Jan, Deng-Yang; Abdo, Suheil F.; Aguilar-Tapia, Antonio; Proux, Olivier; Hazemann, Jean-Louis; Basset, Jean-Marie

    2018-01-01

    Well-defined silica supported bimetallic catalysts Pt100-x Pdx were prepared by Surface Organometallic Chemistry (SOMC) and Ionic-Exchange (IE) methods. For all investigated catalysts, iso-butane reaction with hydrogen under differential conditions led to the formation of methane and propane, n-butane, and traces of iso-butylene. The total reaction rate decreased with increasing the Pd loading for both catalysts series as a result of decreasing turnover rate of both isomerization and hydrogenolysis. In the case of Pt100-x Pdx(SOMC) catalysts, the experimental results in combination with DFT calculations suggested a selective coverage of Pt (1 0 0) surface by agglomerated Pd atoms like “islands”, assuming that each metal roughly keeps its intrinsic catalytic properties with relatively small electron transfer from Pt to Pd in the case of Pt-rich sample and from Pd to Pt in the case of Pd-rich sample. For the PtPd catalysts prepared by IE, the catalytic behavior could be explained by the formation of a surface alloy between Pt and Pd in the case of Pd-rich sample and by the segregation of a small amount of Pd on the surface in the case of Pt-rich sample, as demonstrated by TEM, EXAFS and DFT. The catalytic results were explained by a structure activity relationship based on the proposed mechanism of CH bond and CC bond activation and cleavage for iso-butane hydrogenolysis, isomerization, cracking and dehydrogenation.

  2. Understanding of the structure activity relationship of PtPd bimetallic catalysts prepared by surface organometallic chemistry and ion exchange during the reaction of iso-butane with hydrogen

    KAUST Repository

    Alshareef, Reem Abdul aziz Hamed

    2018-04-25

    Well-defined silica supported bimetallic catalysts Pt100-x Pdx were prepared by Surface Organometallic Chemistry (SOMC) and Ionic-Exchange (IE) methods. For all investigated catalysts, iso-butane reaction with hydrogen under differential conditions led to the formation of methane and propane, n-butane, and traces of iso-butylene. The total reaction rate decreased with increasing the Pd loading for both catalysts series as a result of decreasing turnover rate of both isomerization and hydrogenolysis. In the case of Pt100-x Pdx(SOMC) catalysts, the experimental results in combination with DFT calculations suggested a selective coverage of Pt (1 0 0) surface by agglomerated Pd atoms like “islands”, assuming that each metal roughly keeps its intrinsic catalytic properties with relatively small electron transfer from Pt to Pd in the case of Pt-rich sample and from Pd to Pt in the case of Pd-rich sample. For the PtPd catalysts prepared by IE, the catalytic behavior could be explained by the formation of a surface alloy between Pt and Pd in the case of Pd-rich sample and by the segregation of a small amount of Pd on the surface in the case of Pt-rich sample, as demonstrated by TEM, EXAFS and DFT. The catalytic results were explained by a structure activity relationship based on the proposed mechanism of CH bond and CC bond activation and cleavage for iso-butane hydrogenolysis, isomerization, cracking and dehydrogenation.

  3. Various characteristics of Ni and Pt-Al2O3 nano catalysts prepared by microwave method to be applied in some petrochemical processes

    International Nuclear Information System (INIS)

    Gobara, H.M.; Mohamed, A.R.S.; Khalil, F.H.; El-Shall, M.S.; Hassan, S.A.

    2014-01-01

    Alumina-supported metal nano catalysts were prepared via the microwave method, by loading nano Ni particles (at 1, 3 and 5 wt %) or nano Pt particles (at 0.3, 0.6 and 0.9 wt %). Structural and adsorption features of the nano catalysts were revealed through XRD, DSC- DTA, TEM, H 2 -chemisorption and N 2 -physisorption. N 2 -adsorption-desorption isotherms of type IV were related typically to meso porous materials with H 2 class of hysteresis loops characterizing ink bottle type of pores. The well dispersed nano-sized metal particles were evidenced in the studied catalytic systems, exhibiting marked thermal stability up to 800 degree C. The catalytic performances of different catalyst samples were assessed during cyclohexane, normal hexane and ethanol conversions, using the micro-catalytic pulse technique at different operating conditions. The 5% Ni-γAl 2 O 3 sample was found to be the most active in dehydration of ethanol to produce ethylene, as well as in n -hexane cracking. However, the 1% Ni-Al 2 O 3 sample showed the highest dehydrogenation activity for selective production of benzene from cyclohexane. On the other hand, the 0.9% Pt-γAl 2 O 3 sample exhibited the highest activity in the dehydration of ethanol and in the dehydrogenation of cyclohexane. The 0.3% Pt-γAl 2 O 3 sample was the most active in the dehydrocyclization of normal hexane, as compared to the other catalyst samples under study

  4. 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.

  5. Modulation of spin-orbit torque efficiency by thickness control of heavy metal layers in Co/Pt multilayers

    Energy Technology Data Exchange (ETDEWEB)

    Sethi, P.; Krishnia, S.; Li, S.H.; Lew, W.S., E-mail: wensiang@ntu.edu.sg

    2017-03-15

    We investigate and quantify spin-orbit torque (SOT) strength by current induced effective in-plane magnetic fields and spin Hall angle (SHA) using AC harmonic Hall voltage measurements techniques on Ta/Pt/Co/Pt/Co/Ta thin film structures. The proposed Co/Pt thin film double stack gives property enhancement on thermal stability and perpendicular magnetization anisotropy strength over the single stack Pt/Co/Ta. In the proposed Co/Pt double stack we observed that increasing the Ta capping thickness to three times enhances the SHA in similar order, consistent with larger spin injection efficiency. Doubling the Pt spacer layer thickness reduces the SHA by nearly 1.4 times, due to partial cancellation of SOT by bottom layer Pt, negating the increase from the top Co/Pt interface. The in-plane current threshold for magnetization switching is lower with the increase of the SHA.

  6. Exceptionally Stable and Efficient Solid Supported Hoveyda-Type Catalyst

    Czech Academy of Sciences Publication Activity Database

    Skowerski, K.; Pastva, J.; Czarnocki, S. J.; Janošcová, Jana

    2015-01-01

    Roč. 19, č. 7 (2015), s. 872-877 ISSN 1083-6160 Institutional support: RVO:61388955 Keywords : OLEFIN-METATHESIS CATALYSTS * RING-CLOSING METATHESIS * N-HETEROCYCLIC CARBENES Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.922, year: 2015

  7. An efficient polymeric micromotor doped with Pt nanoparticle@carbon nanotubes for complex bio-media.

    Science.gov (United States)

    Li, Yana; Wu, Jie; Xie, Yuzhe; Ju, Huangxian

    2015-04-14

    A highly efficient polymeric tubular micromotor doped with Pt nanoparticle@carbon nanotubes is fabricated by template-assisted electrochemical growth. The micromotors preserve good navigation in multi-media and surface modification, along with simple synthesis, easy functionalization and good biocompatibility, displaying great promise in biological applications.

  8. Fabrication of Nonenzymatic Glucose Sensors Based on Multiwalled Carbon Nanotubes with Bimetallic Pt-M (M = Ru and Sn Catalysts by Radiolytic Deposition

    Directory of Open Access Journals (Sweden)

    Sun-Young Kwon

    2012-01-01

    Full Text Available Nonenzymatic glucose sensors employing multiwalled carbon nanotubes (MWNTs with highly dispersed Pt-M (M = Ru and Sn nanoparticles (Pt-M@PVP-MWNTs were fabricated by radiolytic deposition. The Pt-M nanoparticles on the MWNTs were characterized by transmittance electron microscopy, elemental analysis, and X-ray diffraction. They were found to be well dispersed and to exhibit alloy properties on the MWNT support. Electrochemical testing showed that these nonenzymatic sensors had larger currents (mA than that of a bare glassy carbon (GC electrode and one modified with MWNTs. The sensitivity (A mM−1, linear range (mM, and detection limit (mM (S/N = 3 of the glucose sensor with the Pt-Ru catalyst in NaOH electrolyte were determined as 18.0, 1.0–2.5, 0.7, respectively. The corresponding data of the sensor with Pt-Sn catalyst were 889.0, 1.00–3.00, and 0.3, respectively. In addition, these non-enzymatic sensors can effectively avoid interference arising from the oxidation of the common interfering species ascorbic acid and uric acid in NaOH electrolyte. The experimental results show that such sensors can be applied in the detection of glucose in commercial red wine samples.

  9. Catalytic Hydrogenation and Hydrodeoxygenation of Furfural over Pt(111): A Model System for the Rational Design and Operation of Practical Biomass Conversion Catalysts.

    Science.gov (United States)

    Taylor, Martin J; Jiang, Li; Reichert, Joachim; Papageorgiou, Anthoula C; Beaumont, Simon K; Wilson, Karen; Lee, Adam F; Barth, Johannes V; Kyriakou, Georgios

    2017-04-20

    Furfural is a key bioderived platform chemical whose reactivity under hydrogen atmospheres affords diverse chemical intermediates. Here, temperature-programmed reaction spectrometry and complementary scanning tunneling microscopy (STM) are employed to investigate furfural adsorption and reactivity over a Pt(111) model catalyst. Furfural decarbonylation to furan is highly sensitive to reaction conditions, in particular, surface crowding and associated changes in the adsorption geometry: furfural adopts a planar geometry on clean Pt(111) at low coverage, tilting at higher coverage to form a densely packed furfural adlayer. This switch in adsorption geometry strongly influences product selectivity. STM reveals the formation of hydrogen-bonded networks for planar furfural, which favor decarbonylation on clean Pt(111) and hydrogenolysis in the presence of coadsorbed hydrogen. Preadsorbed hydrogen promotes furfural hydrogenation to furfuryl alcohol and its subsequent hydrogenolysis to methyl furan, while suppressing residual surface carbon. Furfural chemistry over Pt is markedly different from that over Pd, with weaker adsorption over the former affording a simpler product distribution than the latter; Pd catalyzes a wider range of chemistry, including ring-opening to form propene. Insight into the role of molecular orientation in controlling product selectivity will guide the design and operation of more selective and stable Pt catalysts for furfural hydrogenation.

  10. The Use of C-MnO2 as Hybrid Precursor Support for a Pt/C-MnxO1+x Catalyst with Enhanced Activity for the Methanol Oxidation Reaction (MOR

    Directory of Open Access Journals (Sweden)

    Alessandro H.A. Monteverde Videla

    2015-07-01

    Full Text Available Platinum (Pt nanoparticles are deposited on a hybrid support (C-MnO2 according to a polyol method. The home-made catalyst, resulted as Pt/C-MnxO1+x, is compared with two different commercial platinum based materials (Pt/C and PtRu/C. The synthesized catalyst is characterized by means of FESEM, XRD, ICP-MS, XPS and μRS analyses. MnO2 is synthesized and deposited over a commercial grade of carbon (Vulcan XC72 by facile reduction of potassium permanganate in acidic solution. Pt nanoparticles are synthesized on the hybrid support by a polyol thermal assisted method (microwave irradiation, followed by an annealing at 600 °C. The obtained catalyst displays a support constituted by a mixture of manganese oxides (Mn2O3 and Mn3O4 with a Pt loading of 19 wt. %. The electro-catalytic activity towards MOR is assessed by RDE in acid conditions (0.5 M H2SO4, evaluating the ability to oxidize methanol in 1 M concentration. The synthesized Pt/C-MnxO1+x catalyst shows good activity as well as good stability compared to the commercial Pt/C based catalyst.

  11. One-pot solvothermal synthesis of ordered intermetallic Pt2In3 as stable and efficient electrocatalyst towards direct alcohol fuel cell application

    Science.gov (United States)

    Jana, Rajkumar; Peter, Sebastian C.

    2016-10-01

    Ordered intermetallic Pt2In3 nanoparticles have been synthesized by superhydride reduction of K2PtCl4 and InCl3.xH2O precursors using facile, one-pot solvothermal method. We report surfactant free solvothermal synthesis of a novel ordered Pt2In3 intermetallic nanoparticles for the first time. The structure and morphology of the catalyst has been confirmed by powder X-ray diffraction, transmission electron microscopy, field emission scanning electron microscopy, energy-dispersive spectrometry and X-ray photoelectron spectroscopy. The electrocatalytic properties of the catalysts have been investigated by cyclic voltammetry and chronoamperometry. The as prepared Pt2In3 catalyst exhibit far superior electrocatalytic activity and stability towards alcohol oxidation over commercial Pt/C. The specific activity of as synthesized catalyst was found to be 3.2 and 2.3 times higher than commercial Pt/C for methanol and ethanol oxidation, respectively. This improved activity and durability of the Pt2In3 nanoparticles can make the catalyst an ideal catalyst candidate for direct alcohol fuel cell.

  12. Efficient Air Desulfurization Catalysts Derived from Pig Manure Liquefaction Char

    Directory of Open Access Journals (Sweden)

    Rajiv Wallace

    2017-11-01

    Full Text Available Biochar from the liquefaction of pig manure was used as a precursor of H2S desulfurization adsorbents. In its inorganic matter, it contains marked quantities of calcium, magnesium and iron, which are known as hydrogen sulfide oxidation catalysts. The char was used either as-received or mixed with 10% nanographite. The latter was added to increase both the content of the carbon phase and conductivity. ZnCl2 in two different ratios of char to an activation agent (1:1 and 1:2 was used to create the porosity in the carbon phase. The content of the later was between 18–45%. The activated samples adsorbed 144 mg/g H2S. Sulfur was the predominant product of reactive adsorption. Its deposition in the pore system and blockage of the most active pores ceased the materials’ activity. The presence of the catalytic phase was necessary but not sufficient to guarantee good performance. The developed porosity, which can store oxidation products in the resulting composite, is essential for the good performance of the desulfurization process. The surface of the composite with nanographite showed the highest catalytic activity, similar to that of the commercial Midas® carbon catalyst. The results obtained indicate that a high quality reactive adsorbent/catalyst for H2S removal can be obtained from pig manure liquefaction wastes.

  13. Catalysts macroporosity and their efficiency in sulphur sub-dew point Claus tail gas treating processes

    Energy Technology Data Exchange (ETDEWEB)

    Tsybulevski, A.M.; Pearson, M. [Alcoa Industrial Chemicals, 16010 Barker`s Point Lane, Houston, TX (United States); Morgun, L.V.; Filatova, O.E. [All-Russian Research Institute of Natural Gases and Gas Technologies VNIIGAZ, Moscow (Russian Federation); Sharp, M. [Porocel Corporation, Westheimer, Houston, TX (United States)

    1996-10-08

    The efficiency of 4 samples of alumina catalyst has been studied experimentally in the course of the Claus `tail gas` treating processes at the sulphur sub-dew point (TGTP). The samples were characterized by the same chemical and crystallographic composition, the same volume of micropores, the same surface area and the same catalytic activity but differed appreciably in the volume of macropores. An increase in the effective operation time of the catalysts before breakthrough of unrecoverable sulphur containing compounds, with the increasing macropore volume has been established. A theoretical model of the TGTP has been considered and it has been shown that the increase in the sulphur capacity of the catalysts with a larger volume of macropores is due to an increase in the catalysts efficiency factor and a slower decrease in their diffusive permeability during filling of micropores by sulphur

  14. Magnetic nanoparticle supported phosphotungstic acid: An efficient catalyst for the synthesis of xanthene derivatives

    Science.gov (United States)

    Patel, Nipun; Katheriya, Deepak; Dadhania, Harsh; Dadhania, Abhishek

    2018-05-01

    Magnetic nanoparticle supported phosphotungstic acid (Fe3O4@SiO2-HPW) was applied as a highly efficient catalyst for the synthesis of 14H-dibenzoxanthene derivatives via condensation reaction of 2-naphthol and aryl aldehydes. The catalyst was found highly efficient for the synthesis of xanthene derivatives under solvent free condition. The catalyst showed high activity and stability during the reaction and provided excellent yield of the corresponding products in short reaction time. All the synthesized compounds were characterized through FT-IR, 1H-NMR and 13C-NMR spectroscopic techniques. Furthermore, the catalyst is magnetically recoverable and can be reused several times without significant loss of its catalytic activity.

  15. Synthesis and Characterization of Pt-loaded carbon nanostructures derived from polyaniline nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Gong Da; Kim, Pil; Lee, Youn Sik [Div. of Chemical Engineering, Nanomaterials Processing Research Center, Chonbuk NationalUniversity, Jeonju (Korea, Republic of)

    2017-03-15

    Proton exchange membrane fuel cells (PEMFC) are one of the most advanced fuel cells for future energy, owing to their high conversion efficiency, quick start-up, rapid response to variable loading, and relatively low operating temperature, compared with of her conventional energy conversion devices. PANTs were synthesized to have various aspect ratios and inner diameters. As the aniline concentration increased, the PANTs’ inner diameter greatly decreased, but their outer diameters only slightly increased, leading to a decrease in their aspect ratios. Carbonization of PANTs resulted in the formation of corresponding CNSs. Pt nanoparticles were successfully formed on the CNSs under N{sub 2} or N{sub 2}/NH{sub 3} flow. The Pt nanoparticles of the Pt- CNS-N{sub 2} /NH{sub 3} catalysts were smaller in size, less aggregated, and more uniformly dispersed than those of the Pt- CNS-N{sub 2} catalysts. The ECSA values of Pt-CNS-N{sub 2} /NH{sub 3} were larger than those of Pt-CNS-N{sub 2} and Pt/C. The half wave potentials of the Pt-CNS-N{sub 2} catalysts were lower than those of the Pt-CNS-N{sub 2} /NH{sub 3} , and close to those of the Pt/C. The Pt-CNS-N{sub 2} /NH{sub 3} catalysts exhibited better kinetic performance than the Pt-CNS -N{sub 2} catalysts and Pt/C.

  16. Electronic structure of Pt-Co cathode catalysts in membrane electrolyte assembly observed by X-ray absorption fine structure spectroscopy with different probing depth

    International Nuclear Information System (INIS)

    Kobayashi, M.; Hidai, S.; Niwa, H.; Harada, Y.; Oshima, M.; Ofuchi, H.; Nakamori, Y.; Aoki, T.

    2010-01-01

    Electronic structures of Pt-Co cathode and Pt-Ru anode catalysts in membrane electrolyte assemblies (MEAs) for polymer electrolyte fuel cell have been investigated using X-ray absorption near edge structure (XANES) spectroscopy, and the changes of electronic structures accompanied with degradation have been observed by comparison between spectra obtained by fluorescence-yield (FY) and conversion-electron-yield (CEY) methods, probing depths of which are several hundreds μm and ∼100 nm, respectively. The Co K XANES spectra of the as-fabricated MEA show that the Co atoms in the cathode are metallic and oxidized Co ions exist at the interface between the cathode and electrolyte. The spectra of the long-time operated MEA suggest that the oxidation of Co makes progress with degradation of the cathode catalysts. In contrast to the Co K XANES spectra, the line shape of the Ru K XANES spectra is unchanged even after the long-time operation.

  17. A Highly Efficient Catalyst for Oxime Ligation and Hydrazone-Oxime Exchange Suitable for Bioconjugation

    OpenAIRE

    Rashidian, Mohammad; Mahmoodi, Mohammad M.; Shah, Rachit; Dozier, Jonathan K.; Wagner, Carston R.; Distefano, Mark D.

    2013-01-01

    Imine-based reactions are useful for a wide range of bioconjugation applications. Although aniline is known to catalyze the oxime ligation reaction under physiological conditions, it suffers from slow reaction kinetics, specifically when a ketone is being used or when hydrazone-oxime exchange is performed. Here, we report on the discovery of a new catalyst that is up to 15 times more efficient than aniline. That catalyst, m-phenylenediamine (mPDA), was initially used to analyze the kinetics o...

  18. Preparation of the Pt/CNTs Catalyst and Its Application to the Fabrication of Hydrogenated Soybean Oil Containing a Low Content of Trans Fatty Acids Using the Solid Polymer Electrolyte Reactor.

    Science.gov (United States)

    Zheng, Huanyu; Ding, Yangyue; Xu, Hui; Zhang, Lin; Cui, Yueting; Han, Jianchun; Zhu, Xiuqing; Yu, Dianyu; Jiang, Lianzhou; Liu, Lilai

    2018-08-01

    Pt/CNTs were synthesized with an ethylene glycol reduction method, and the effects of carboxyl functionalization, ultrasonic power and the concentration of chloroplatinic acid on the catalytic activity of Pt/CNTs were investigated. The optimal performance of the Pt/CNTs catalyst was obtained when the ultrasonic power was 300 W and the concentration of chloroplatinic acid was 40 mg/mL. The durability and stability of the Pt/CNTs catalyst were considerably better compared to Pt/C, as shown by cyclic voltammetry measurement results. The trans fatty acids content of the obtained hydrogenated soybean oil (IV: 108.4 gl2/100 g oil) using Pt/CNTs as the cathode catalyst in a solid polymer electrolyte reactor was only 1.49%. The IV of hydrogenated soybean oil obtained using CNTs as carrier with Pt loading 0.1 mg/cm2 (IV: 108.4 gl2/100 g oil) was lower than carbon with a Pt loading of 0.8 mg/cm2 (IV: 109.9 gl2/100 g oil). Thus, to achive the same IV, the usage of Pt was much less when carbon nanotubes were selected as catalyst carrier compared to traditional carbon carrier. The changes of fatty acid components and the hydrogenated selectivity of octadecenoic acid were also discussed.

  19. Fischer-Tropsch synthesis: study of the promotion of Pt on the reduction property of Co/Al2O3 catalysts by in situ EXAFS of Co K and Pt LIII edges and XPS

    International Nuclear Information System (INIS)

    Jacobs, G.; Chaney, J.A.; Patterson, P.M.; Das, T.K.; Maillot, J.C.; Davis, B.H.

    2004-01-01

    The addition of platinum metal to cobalt/alumina-based Fischer-Tropsch synthesis (FTS) catalysts increases both the reduction rate and, consequently, the density of active cobalt sites. Platinum also lowers the temperature of the two-step conversion of cobalt oxide to cobalt metal observed in temperature programmed reduction (TPR) as Co 3 O 4 to CoO and CoO to Co 0 . The interaction of the alumina support with cobalt oxide ultimately determines the active site density of the catalyst surface. This interaction can be controlled by varying the cobalt loading and dispersion, selecting supports with differing surface areas or pore sizes, or changing the noble metal promoter. However, the active site density is observed to depend primarily on the cluster size and extent of reduction, and there is a direct relationship between site density and FTS rate. In this work, in situ extended X-ray absorption fine structure (EXAFS) at the L III edge of Pt was used to show that isolated Pt atoms interact with supported cobalt clusters without forming observable Pt-Pt bonds. K-edge EXAFS was also used to verify that the cobalt cluster size increases slightly for those systems with Pt promotion. X-ray absorption near-edge spectroscopy (XANES) was used to examine the remaining cobalt clusters after the first stage of TPR, and it revealed that the species were almost entirely cobalt (II) oxide. After the second stage of TPR to form cobalt metal, a residual oxide persists in the sample, and this oxide has been identified as cobalt (II) aluminate using X-ray photoelectron spectroscopy (XPS). Sequential in situ reduction of promoted and unpromoted systems was also monitored through XPS, and Pt was seen to increase the extent of cobalt reduction by a factor of two. (orig.)

  20. Carbohydrates as efficient catalysts for the hydration of α-amino nitriles.

    Science.gov (United States)

    Chitale, Sampada; Derasp, Joshua S; Hussain, Bashir; Tanveer, Kashif; Beauchemin, André M

    2016-11-01

    Directed hydration of α-amino nitriles was achieved under mild conditions using simple carbohydrates as catalysts exploiting temporary intramolecularity. A broadly applicable procedure using both formaldehyde and NaOH as catalysts efficiently hydrated a variety of primary and secondary susbtrates, and allowed the hydration of enantiopure substrates to proceed without racemization. This work also provides a rare comparison of the catalytic activity of carbohydrates, and shows that the simple aldehydes at the basis of chemical evolution are efficient organocatalysts mimicking the function of hydratase enzymes. Optimal catalytic efficiency was observed with destabilized aldehydes, and with difficult substrates only simple carbohydrates such as formaldehyde and glycolaldehyde proved reliable.

  1. Optimization of the reaction parameters of heavy naphtha reforming process using Pt-Re/Al2O3 catalyst system

    Directory of Open Access Journals (Sweden)

    Hussien A. Elsayed

    2017-12-01

    Full Text Available One of the most significant procedures in oil refineries is naphtha catalytic reforming unit in which high octane gasoline is gained. Normally, in oil refineries, flow instability in the composition of feedstock can affect the product quality. The aim of the present work was focused on modifications of the final product flow rate and product’s octane number with respect to the modifications of the feedstock composition. The main three reforming reactions investigated, namely; dehydrogenation, dehydrocyclization, and hydrocracking were conducted employing silica supported bimetallic (Pt-Re patented catalyst. Optimization of the catalytic process reaction conditions, i.e.; temperature, hydrogen pressure and liquid hourly space velocity (LHSV was carried out with regard to conversion and selectivity. The optimization results indicated that heavy naphtha component conversion (paraffin’s and naphthenes increases with an increasing in reaction temperature and pressure while decreases with an increase in LHSV. The kinetic study of catalytic reforming reactions reported helped establishing the reaction model explicitly.

  2. In situ NAP-XPS spectroscopy during methane dry reforming on ZrO2/Pt(1 1 1) inverse model catalyst

    Science.gov (United States)

    Rameshan, C.; Li, H.; Anic, K.; Roiaz, M.; Pramhaas, V.; Rameshan, R.; Blume, R.; Hävecker, M.; Knudsen, J.; Knop-Gericke, A.; Rupprechter, G.

    2018-07-01

    Due to the need of sustainable energy sources, methane dry reforming is a useful reaction for conversion of the greenhouse gases CH4 and CO2 to synthesis gas (CO  +  H2). Syngas is the basis for a wide range of commodity chemicals and can be utilized for fuel production via Fischer–Tropsch synthesis. The current study focuses on spectroscopic investigations of the surface and reaction properties of a ZrO2/Pt inverse model catalyst, i.e. ZrO2 particles (islands) grown on a Pt(1 1 1) single crystal, with emphasis on in situ near ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) during MDR reaction. In comparison to technological systems, model catalysts facilitate characterization of the surface (oxidation) state, surface adsorbates, and the role of the metal-support interface. Using XPS and infrared reflection absorption spectroscopy we demonstrated that under reducing conditions (UHV or CH4) the ZrO2 particles transformed to an ultrathin ZrO2 film that started to cover (wet) the Pt surface in an SMSI-like fashion, paralleled by a decrease in surface/interface oxygen. In contrast, (more oxidizing) dry reforming conditions with a 1:1 ratio of CH4 and CO2 were stabilizing the ZrO2 particles on the model catalyst surface (or were even reversing the strong metal support interaction (SMSI) effect), as revealed by in situ XPS. Carbon deposits resulting from CH4 dissociation were easily removed by CO2 or by switching to dry reforming conditions (673–873 K). Thus, at these temperatures the active Pt surface remained free of carbon deposits, also preserving the ZrO2/Pt interface.

  3. Controlled surface segregation leads to efficient coke-resistant nickel/platinum bimetallic catalysts for the dry reforming of methane

    KAUST Repository

    Li, Lidong; Zhou, Lu; Ould-Chikh, Samy; Anjum, Dalaver; Kanoun, Mohammed; Scaranto, Jessica; Hedhili, Mohamed Nejib; Khalid, Syed; Laveille, Paco; D'Souza, Lawrence; Clo, Alain M.; Basset, Jean-Marie

    2015-01-01

    Surface composition and structure are of vital importance for heterogeneous catalysts, especially for bimetallic catalysts, which often vary as a function of reaction conditions (known as surface segregation). The preparation of bimetallic catalysts with controlled metal surface composition and structure is very challenging. In this study, we synthesize a series of Ni/Pt bimetallic catalysts with controlled metal surface composition and structure using a method derived from surface organometallic chemistry. The evolution of the surface composition and structure of the obtained bimetallic catalysts under simulated reaction conditions is investigated by various techniques, which include CO-probe IR spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, extended X-ray absorption fine structure analysis, X-ray absorption near-edge structure analysis, XRD, and X-ray photoelectron spectroscopy. It is demonstrated that the structure of the bimetallic catalyst is evolved from Pt monolayer island-modified Ni nanoparticles to core-shell bimetallic nanoparticles composed of a Ni-rich core and a Ni/Pt alloy shell upon thermal treatment. These catalysts are active for the dry reforming of methane, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure. The reform of reforming: A series of alumina-supported Ni/Pt bimetallic nanoparticles (NPs) with controlled surface composition and structure are prepared. Remarkable surface segregation for these bimetallic NPs is observed upon thermal treatment. These bimetallic NPs are active catalysts for CO2 reforming of CH4, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure.

  4. Controlled surface segregation leads to efficient coke-resistant nickel/platinum bimetallic catalysts for the dry reforming of methane

    KAUST Repository

    Li, Lidong

    2015-02-03

    Surface composition and structure are of vital importance for heterogeneous catalysts, especially for bimetallic catalysts, which often vary as a function of reaction conditions (known as surface segregation). The preparation of bimetallic catalysts with controlled metal surface composition and structure is very challenging. In this study, we synthesize a series of Ni/Pt bimetallic catalysts with controlled metal surface composition and structure using a method derived from surface organometallic chemistry. The evolution of the surface composition and structure of the obtained bimetallic catalysts under simulated reaction conditions is investigated by various techniques, which include CO-probe IR spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, extended X-ray absorption fine structure analysis, X-ray absorption near-edge structure analysis, XRD, and X-ray photoelectron spectroscopy. It is demonstrated that the structure of the bimetallic catalyst is evolved from Pt monolayer island-modified Ni nanoparticles to core-shell bimetallic nanoparticles composed of a Ni-rich core and a Ni/Pt alloy shell upon thermal treatment. These catalysts are active for the dry reforming of methane, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure. The reform of reforming: A series of alumina-supported Ni/Pt bimetallic nanoparticles (NPs) with controlled surface composition and structure are prepared. Remarkable surface segregation for these bimetallic NPs is observed upon thermal treatment. These bimetallic NPs are active catalysts for CO2 reforming of CH4, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure.

  5. Metamorphosis of the mixed phase PtRu anode catalyst for direct methanol fuel cells after exposure of methanol: In situ and ex situ characterizations

    Energy Technology Data Exchange (ETDEWEB)

    Chakraborty, Debasish [Center for Individual Nanoparticle Functionality (CINF), Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Aerosol Laboratory, Nano.DTU, Department of Chemical Engineering, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Chorkendorff, Ib [Center for Individual Nanoparticle Functionality (CINF), Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Department of Physics, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Johannessen, Tue [Aerosol Laboratory, Nano.DTU, Department of Chemical Engineering, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark)

    2007-11-08

    The change in the mixed phase heavily oxidized PtRu anode with the exposure of methanol in a direct methanol fuel cell (DMFC) has been investigated by electrochemical impedance spectroscopy (EIS) and X-ray diffraction (XRD). The investigation had two major objectives: (i) to explore the original state of the active catalyst and (ii) to understand if alloying of Pt and Ru is a requirement for higher methanol oxidation activity. It was found that the methanol oxidation activity gradually improved for {proportional_to}2 h of exposure. The impedance spectra were taken at different times within this time of improvement of activity. The impedance spectra were deconvoluted in different contributions like membrane resistance (R{sub m}), charge transfer resistance (R{sub Ct}), adsorption resistance (R{sub ad}), and oxidation resistance (R{sub ox}). The improvement of the activity was explained in terms of the effect of the pretreatment on different contributions. XRD was done on the virgin and methanol exposed sample as a possible mean to identify the difference. It was postulated that the reduction of the as prepared PtRu after exposure was responsible for the activity improvement. Also, it was shown that bulk alloy formation is not a necessary condition for higher methanol activity of PtRu catalysts. (author)

  6. Biosourced polymetallic catalysts: an efficient means to synthesize underexploited platform molecules from carbohydrates.

    Science.gov (United States)

    Escande, Vincent; Olszewski, Tomasz K; Petit, Eddy; Grison, Claude

    2014-07-01

    Polymetallic hyperaccumulating plants growing on wastes from former mining activity were used as the starting material in the preparation of novel plant-based Lewis acid catalysts. The preparation of biosourced Lewis acid catalysts is a new way to make use of mining wastes. These catalysts were characterized by X-ray fluorescence, X-ray diffraction, inductively coupled plasma mass spectrometry, and direct infusion electrospray ionization mass spectrometry. These analyses revealed a complex composition of metal species, present mainly as polymetallic chlorides. The catalysts proved to be efficient and recyclable in a solid-state version of the Garcia Gonzalez reaction, which has been underexploited until now in efforts to use carbohydrates from biomass. This methodology was extended to various carbohydrates to obtain the corresponding polyhydroxyalkyl furans in 38-98% yield. These plant-based catalysts may be a better alternative to classical Lewis acid catalysts that were previously used for the Garcia Gonzalez reaction, such as ZnCl2 , FeCl3 , and CeCl3 , which are often unrecyclable, require aqueous treatments, or rely on metals, the current known reserves of which will be consumed in the coming decades. Moreover, the plant-based catalysts allowed novel control of the Garcia Gonzalez reaction, as two different products were obtained depending on the reaction conditions. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. Facile Synthesis of Quasi-One-Dimensional Au/PtAu Heterojunction Nanotubes and Their Application as Catalysts in an Oxygen-Reduction Reaction.

    Science.gov (United States)

    Cai, Kai; Liu, Jiawei; Zhang, Huan; Huang, Zhao; Lu, Zhicheng; Foda, Mohamed F; Li, Tingting; Han, Heyou

    2015-05-11

    An intermediate-template-directed method has been developed for the synthesis of quasi-one-dimensional Au/PtAu heterojunction nanotubes by the heterogeneous nucleation and growth of Au on Te/Pt core-shell nanostructures in aqueous solution. The synthesized porous Au/PtAu bimetallic nanotubes (PABNTs) consist of porous tubular framework and attached Au nanoparticles (AuNPs). The reaction intermediates played an important role in the preparation, which fabricated the framework and provided a localized reducing agent for the reduction of the Au and Pt precursors. The Pt7 Au PABNTs showed higher electrocatalytic activity and durability in the oxygen-reduction reaction (ORR) in 0.1 M HClO4 than porous Pt nanotubes (PtNTs) and commercially available Pt/C. The mass activity of PABNTs was 218 % that of commercial Pt/C after an accelerated durability test. This study demonstrates the potential of PABNTs as highly efficient electrocatalysts. In addition, this method provides a facile strategy for the synthesis of desirable hetero-nanostructures with controlled size and shape by utilizing an intermediate template. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  8. Ethanol electrooxidation on a carbon-supported Pt catalyst at elevated temperature and pressure: A high-temperature/high-pressure DEMS study

    Energy Technology Data Exchange (ETDEWEB)

    Sun, S.; Halseid, M. Chojak; Heinen, M.; Jusys, Z.; Behm, R.J. [Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm (Germany)

    2009-05-01

    The electrooxidation of ethanol on a Pt/Vulcan catalyst was investigated in model studies by on-line differential electrochemical mass spectrometry (DEMS) over a wide range of reaction temperatures (23-100 C). Potentiodynamic and potentiostatic measurements of the Faradaic current and the CO{sub 2} formation rate, performed at 3 bar overpressure under well-defined transport and diffusion conditions reveal significant effects of temperature, potential and ethanol concentration on the total reaction activity and on the selectivity for the pathway toward complete oxidation to CO{sub 2}. The latter pathway increasingly prevails at higher temperature, lower concentration and lower potentials ({proportional_to}90% current efficiency for CO{sub 2} formation at 100 C, 0.01 M, 0.48 V), while at higher ethanol concentrations (0.1 M), higher potentials or lower temperatures the current efficiency for CO{sub 2} formation drops, reaching values of a few percent at room temperature. These trends result in a significantly higher apparent activation barrier for complete oxidation to CO{sub 2} (68 {+-} 2 kJ mol{sup -1} at 0.48 V, 0.1 M) compared to that of the overall ethanol oxidation reaction determined from the Faradaic current (42 {+-} 2 kJ mol{sup -1} at 0.48 V, 0.1 M). The mechanistic implications of these results and the importance of relevant reaction and mass transport conditions in model studies for reaction predictions in fuel cell applications are discussed. (author)

  9. Synthesis and characterization of highly efficient and stable Pr6O11/Ag3PO4/Pt ternary hybrid structure

    International Nuclear Information System (INIS)

    Deng, Jiatao; Liu, Lin; Niu, Tongjun; Sun, Xiaosong

    2017-01-01

    Highlights: • Visible-light-driven Pr 6 O 11 /Ag 3 PO 4 /Pt photocatalysts were prepared. • Pr 6 O 11 /Ag 3 PO 4 /Pt showed highly efficient and stable photocatalystic activity. • The photocatalytic mechanism of Pr 6 O 11 /Ag 3 PO 4 /Pt composite was given. - Abstract: Ag 3 PO 4 is an excellent photocatalyst with high efficiency and quantum yield, but suffers from the fast recombination of photogenerated electron-hole pairs and photo-corrosion. Hereby, the highly efficient and stable visible-light-driven Pr 6 O 11 /Ag 3 PO 4 /Pt photocatalyst were prepared via a three-step wet chemical approach. The as-prepared Pr 6 O 11 /Ag 3 PO 4 /Pt composite was characterized by X-ray diffraction, US-vis diffuse reflectance spectroscopy, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, photoluminescence spectra and transient photocurrent as well. Comparing with single Pr 6 O 11 or Ag 3 PO 4 , the prepared Pr 6 O 11 /Ag 3 PO 4 /Pt composite exhibited much higher photocatalytic activity and stability for the degradation of Rhodamine B under visible light irradiation (>420 nm). The enhanced photocatalytic performance of Pr 6 O 11 /Ag 3 PO 4 /Pt composite has been attributed to the efficient separation of photo-generated electron-hole pairs through a scheme system composed of Pr 6 O 11, Ag 3 PO 4 and Pt.

  10. Visible-light-induced hydrogen production over Pt-Eosin Y catalysts with high surface area silica gel as matrix

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Xiaojie [State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, The Chinese Academy of Sciences, Lanzhou 730000 (China); Graduate University of the Chinese Academy of Sciences, Beijing 100101 (China); Jin, Zhiliang; Li, Shuben; Lu, Gongxuan [State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, The Chinese Academy of Sciences, Lanzhou 730000 (China); Li, Yuexiang [Department of Chemistry, Nanchang University, Nanjing Road 245, Nanchang, 330047 (China)

    2007-03-30

    A new system for the production of hydrogen, constructed using silica gel as a matrix, Eosin Y as a photosensitizer, and Pt as a cocatalyst, has been reported. It was found that the rate of photosensitized hydrogen evolution in the presence of silica gel is enhanced about 10-fold relative to the homogeneous phase, i.e. in the absence of silica gel. The pH value of the solution and the concentration of Eosin Y have remarkable effects on the rate of hydrogen evolution. The optimal pH and concentration of Eosin Y are 7 and 3.60 x 10{sup -4} mol dm{sup -3} (E/S = 1/3) to 7.24 x 10{sup -4} mol dm{sup -3} (E/S = 1/1), respectively. Triethanolamine (TEOA) as an electron donor, the rate of hydrogen evolution and the apparent quantum efficiency in the silica gel system under visible-light irradiation ({lambda} {>=} 420 nm) can reach about 43 {mu}mol h{sup -1} and 10.4%, respectively. In addition, the roles of silica gel, Pt and TEOA, respectively; and the probable mechanism of photosensitized hydrogen evolution have been discussed. (author)

  11. Visible-light-induced hydrogen production over Pt-Eosin Y catalysts with high surface area silica gel as matrix

    Science.gov (United States)

    Zhang, Xiaojie; Jin, Zhiliang; Li, Yuexiang; Li, Shuben; Lu, Gongxuan

    A new system for the production of hydrogen, constructed using silica gel as a matrix, Eosin Y as a photosensitizer, and Pt as a cocatalyst, has been reported. It was found that the rate of photosensitized hydrogen evolution in the presence of silica gel is enhanced about 10-fold relative to the homogeneous phase, i.e. in the absence of silica gel. The pH value of the solution and the concentration of Eosin Y have remarkable effects on the rate of hydrogen evolution. The optimal pH and concentration of Eosin Y are 7 and 3.60 × 10 -4 mol dm -3 (E/S = 1/3) to 7.24 × 10 -4 mol dm -3 (E/S = 1/1), respectively. Triethanolamine (TEOA) as an electron donor, the rate of hydrogen evolution and the apparent quantum efficiency in the silica gel system under visible-light irradiation (λ ≥ 420 nm) can reach about 43 μmol h -1 and 10.4%, respectively. In addition, the roles of silica gel, Pt and TEOA, respectively; and the probable mechanism of photosensitized hydrogen evolution have been discussed.

  12. The catalystic function of leadership in efficient group functioning ...

    African Journals Online (AJOL)

    The more efficient group leaders were found to be more competent and revealed a greater task orientation. Compared to the less efficient groups, the better functioning groups were characterised by a higher degree of shared leadership. The bigger involvement in leadership functions seems to increase the competence ...

  13. Uranous nitrate production for purex process applications using PtO2 catalyst and H2/H2-gas mixtures

    International Nuclear Information System (INIS)

    Sreenivasa Rao, K.; Shyamali, R.; Narayan, C.V.; Patil, A.R.; Jambunathan, U.; Ramanujam, A.; Kansara, V.P.

    2003-04-01

    In the Purex process of spent fuel reprocessing. the twin objectives- decontamination and partitioning are achieved by extracting uranium (VI) and plutonium (IV) together in the solvent 30% TBP-dodecane and then selectively reducing Pu (IV) to Pu (III) in which valency it is least extractable in the solvent. Uranous nitrate stabilized with hydrazine nitrate is the widely employed partitioning agent. The conventional method of producing U(IV) is by the electrolytic reduction of uranyl nitrate with hydrazine nitrate as uranous ion stabilizer. Tre percentage conversion of U(VI) to U(IV) obtained in this method is 50 -60 %. The use of this solution as partitioning agent leads not only to the dilution of the plutonium product but also to increase in uranium processing load by each externally fed uranous nitrate batch. Also the oxide coating of the anode, TSIA (Titanium Substrate Insoluble Anode) wears out after a certain period of operation. This necessitates recoating which is quite cumbersome considering the amount of the decontamination involved. An alternative to the conventional electrolytic method of reduction of uranyl nitrate to uranous nitrate was explored at FRD laboratory .The studies have revealed that near 100% uranous nitrate can be produced by reducing uranyl nitrate with H 2 gas or H 2 (8%)- Ar/N 2 gas mixture in presence of PtO 2 catalyst. This report describes the laboratory scale studies carried out to optimize the various parameters. Based on these studies reduction of uranyl nitrate on a pilot plant scale was carried out. The design and operation of the reductor column and also the various studies carried out in the pilot plant studies are discussed. Near 100% conversion of uranyl nitrate to uranous nitrate and also the redundancy of supply of electrical energy make this process a viable alternative to the existing electrolytic method. (author)

  14. Nanocrystalline Hierarchical ZSM-5: An Efficient Catalyst for the Alkylation of Phenol with Cyclohexene.

    Science.gov (United States)

    Radhika, N P; Selvin, Rosilda; Kakkar, Rita; Roselin, L Selva

    2018-08-01

    In this paper, authors report the synthesis of nanocrystalline hierarchical zeolite ZSM-5 and its application as a heterogeneous catalyst in the alkylation of phenol with cyclohexene. The catalyst was synthesized by vacuum-concentration coupled hydrothermal technique in the presence of two templates. This synthetic route could successfully introduce pores of higher hierarchy in the zeolite ZSM-5 structure. Hierarchical ZSM-5 could catalyse effectively the industrially important reaction of cyclohexene with phenol. We ascribe the high efficiency of the catalyst to its conducive structural features such as nanoscale size, high surface area, presence of hierarchy of pores and existence of Lewis sites along with Brønsted acid sites. The effect of various reaction parameters like duration, catalyst amount, reactant mole ratio and temperature were assessed. Under optimum reaction conditions, the catalyst showed up to 65% selectivity towards the major product, cyclohexyl phenyl ether. There was no discernible decline in percent conversion or selectivity even when the catalyst was re-used for up to four runs. Kinetic studies were done through regression analysis and a mechanistic route based on LHHW model was suggested.

  15. An Efficient Catalyst for the Synthesis of Schiff Bases

    International Nuclear Information System (INIS)

    Fareed, G.; Afza, N.; Kalhoro, M.A.

    2013-01-01

    An efficient high yielding synthesis of Schiff bases (1-17) is derived from condensation of 2-fluorenamine and 4-amino phenol with a variety of aldehydes catalyzed by dodecatungstosilicic acid P/sub 2/O/sub 5/ under solvent free conditions at room temperature. The catayst is found to be more efficient in terms of ease of reaction workup and high yields. This methodology contributes to an energy efficient, facile and environamental friendly synthesis for the preparation of Schiff bases. The structures of afforded Schiff bases were characterized by spectroscopic data and elemental analysis. (author)

  16. Electrochemical study of oxygen reduction reaction in Pt/C catalysts synthesized by photo-deposition; Estudio electroquimico de la reaccion de reduccion de oxigeno en catalizadores de Pt/C sintetizados por fotodeposito

    Energy Technology Data Exchange (ETDEWEB)

    Perez-Galindo, J. A.; Ruiz-Camacho, B.; Valenzuela-Zapata, M. A.; Gonzalez-Huerta, R. G. [IPN, ESIQIE, Mexico, D.F. (Mexico)]. E-mail: rosgonzalez_h@yahoo.com.mx

    2009-09-15

    Fuel batteries are considered one of the principal generators of energy for the immediate future, though their use is limited by their cost and useful lifetime. One of the main components of a fuel battery are electrodes made of a noble metal, such as Pt, dispersed in a support. The interaction between these two components has received a good deal of attention in recent years. It is considered to be responsible for structural growth effects and a decreased dispersion of metal particles on a support, causing the battery to have low overall performance and a reduced useful lifetime. The properties of the support are accentuated in cathode catalysts, where oxygen reduction reactions occur as a result of its operating conditions. Syntheses are currently being investigated to improve the metal-support interaction and thereby increase the lifetime of the fuel battery. This work presents the electrochemical study of nanometric-sized carbon-supported platinum (Pt/C) catalysts synthesized with chemical photo-deposition to determine its catalytic effect and stability for oxygen reduction reaction in an acid medium. C{sub 10}H{sub 14}O{sub 4}Pt (Pt(acac)2) was used as the platinum precursor. The electrochemical study was conducted with cyclic voltamperometry and rotary disc electrode (RDE) techniques, observing that the synthesized catalysts present a behavior similar to that of Pt (E-Tek). The kinetic study showed an open-circuit potential of de 0.96 V with a Tafel slope of 73 mV dec-1, and with a current of 0.1 mA cm-2 the potential is 0.91 V. The authors wish to thank the ICYTDF (project PICS08-37) and the IPN (project SIP-20090433). [Spanish] Las pilas de combustible se perfilan como uno de los principales generadores de energia en un futuro inmediato, pero su utilizacion esta limitada por su costo y tiempo de vida util. Uno de los componentes principales de la pila de combustible son los electrodos integrados por un metal noble, como el Pt, disperso en un soporte. La

  17. 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.

  18. Hydrogen Production by Steam Reforming of Ethanol on Rh-Pt Catalysts: Influence of CeO2, ZrO2, and La2O3 as Supports

    Directory of Open Access Journals (Sweden)

    Bernay Cifuentes

    2015-11-01

    Full Text Available CeO2-, ZrO2-, and La2O3-supported Rh-Pt catalysts were tested to assess their ability to catalyze the steam reforming of ethanol (SRE for H2 production. SRE activity tests were performed using EtOH:H2O:N2 (molar ratio 1:3:51 at a gaseous space velocity of 70,600 h−1 between 400 and 700 °C at atmospheric pressure. The SRE stability of the catalysts was tested at 700 °C for 27 h time on stream under the same conditions. RhPt/CeO2, which showed the best performance in the stability test, also produced the highest H2 yield above 600 °C, followed by RhPt/La2O3 and RhPt/ZrO2. The fresh and aged catalysts were characterized by TEM, XPS, and TGA. The higher H2 selectivity of RhPt/CeO2 was ascribed to the formation of small (~5 nm and stable particles probably consistent of Rh-Pt alloys with a Pt surface enrichment. Both metals were oxidized and acted as an almost constant active phase during the stability test owing to strong metal-support interactions, as well as the superior oxygen mobility of the support. The TGA results confirmed the absence of carbonaceous residues in all the aged catalysts.

  19. Regeneration of LOHC dehydrogenation catalysts: In-situ IR spectroscopy on single crystals, model catalysts, and real catalysts from UHV to near ambient pressure

    International Nuclear Information System (INIS)

    Amende, Max; Kaftan, Andre; Bachmann, Philipp; Brehmer, Richard; Preuster, Patrick; Koch, Marcus

    2016-01-01

    Graphical abstract: - Highlights: • We examine the regeneration of Pt-based catalysts poisoned by LOHC degradation. • A microscopic mechanism of the removal of degradation products from Pt is proposed. • Results of our UHV studies on model catalysts are transferred to real catalysis. • Oxidative regeneration of Pt/alumina is possible under mild conditions (600 K). • The degree and temperature regime of regeneration depends on the catalyst morphology. - Abstract: The Liquid Organic Hydrogen Carrier (LOHC) concept offers an efficient route to store hydrogen using organic compounds that are reversibly hydrogenated and dehydrogenated. One important challenge towards application of the LOHC technology at a larger scale is to minimize degradation of Pt-based dehydrogenation catalysts during long-term operation. Herein, we investigate the regeneration of Pt/alumina catalysts poisoned by LOHC degradation. We combine ultrahigh vacuum (UHV) studies on Pt(111), investigations on well-defined Pt/Al_2O_3 model catalysts, and near-ambient pressure (NAP) measurements on real core–shell Pt/Al_2O_3 catalyst pellets. The catalysts were purposely poisoned by reaction with the LOHC perhydro-dibenzyltoluene (H18-MSH) and with dicyclohexylmethane (DCHM) as a simpler model compound. We focus on oxidative regeneration under conditions that may be applied in real dehydrogenation reactors. The degree of poisoning and regeneration under oxidative reaction conditions was quantified using CO as a probe molecule and measured by infrared reflection-absorption spectroscopy (IRAS) and diffuse reflectance Fourier transform IR spectroscopy (DRIFTS) for planar model systems and real catalysts, respectively. We find that regeneration strongly depends on the composition of the catalyst surface. While the clean surface of a poisoned Pt(111) single crystal is fully restored upon thermal treatment in oxygen up to 700 K, contaminated Pt/Al_2O_3 model catalyst and core–shell pellet were only

  20. Regeneration of LOHC dehydrogenation catalysts: In-situ IR spectroscopy on single crystals, model catalysts, and real catalysts from UHV to near ambient pressure

    Energy Technology Data Exchange (ETDEWEB)

    Amende, Max, E-mail: max.amende@fau.de [Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Kaftan, Andre, E-mail: andre.kaftan@fau.de [Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Bachmann, Philipp, E-mail: philipp.bachmann@fau.de [Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Brehmer, Richard, E-mail: richard.brehmer@fau.de [Lehrstuhl für Chemische Reaktionstechnik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Preuster, Patrick, E-mail: patrick.preuster@fau.de [Lehrstuhl für Chemische Reaktionstechnik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Koch, Marcus, E-mail: marcus.koch@crt.cbi.uni-erlangen.de [Lehrstuhl für Chemische Reaktionstechnik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); and others

    2016-01-01

    Graphical abstract: - Highlights: • We examine the regeneration of Pt-based catalysts poisoned by LOHC degradation. • A microscopic mechanism of the removal of degradation products from Pt is proposed. • Results of our UHV studies on model catalysts are transferred to real catalysis. • Oxidative regeneration of Pt/alumina is possible under mild conditions (600 K). • The degree and temperature regime of regeneration depends on the catalyst morphology. - Abstract: The Liquid Organic Hydrogen Carrier (LOHC) concept offers an efficient route to store hydrogen using organic compounds that are reversibly hydrogenated and dehydrogenated. One important challenge towards application of the LOHC technology at a larger scale is to minimize degradation of Pt-based dehydrogenation catalysts during long-term operation. Herein, we investigate the regeneration of Pt/alumina catalysts poisoned by LOHC degradation. We combine ultrahigh vacuum (UHV) studies on Pt(111), investigations on well-defined Pt/Al{sub 2}O{sub 3} model catalysts, and near-ambient pressure (NAP) measurements on real core–shell Pt/Al{sub 2}O{sub 3} catalyst pellets. The catalysts were purposely poisoned by reaction with the LOHC perhydro-dibenzyltoluene (H18-MSH) and with dicyclohexylmethane (DCHM) as a simpler model compound. We focus on oxidative regeneration under conditions that may be applied in real dehydrogenation reactors. The degree of poisoning and regeneration under oxidative reaction conditions was quantified using CO as a probe molecule and measured by infrared reflection-absorption spectroscopy (IRAS) and diffuse reflectance Fourier transform IR spectroscopy (DRIFTS) for planar model systems and real catalysts, respectively. We find that regeneration strongly depends on the composition of the catalyst surface. While the clean surface of a poisoned Pt(111) single crystal is fully restored upon thermal treatment in oxygen up to 700 K, contaminated Pt/Al{sub 2}O{sub 3} model catalyst and

  1. Recent Advances on Electro-Oxidation of Ethanol on Pt- and Pd-Based Catalysts: From Reaction Mechanisms to Catalytic Materials

    Directory of Open Access Journals (Sweden)

    Ye Wang

    2015-09-01

    Full Text Available The ethanol oxidation reaction (EOR has drawn increasing interest in electrocatalysis and fuel cells by considering that ethanol as a biomass fuel has advantages of low toxicity, renewability, and a high theoretical energy density compared to methanol. Since EOR is a complex multiple-electron process involving various intermediates and products, the mechanistic investigation as well as the rational design of electrocatalysts are challenging yet essential for the desired complete oxidation to CO2. This mini review is aimed at presenting an overview of the advances in the study of reaction mechanisms and electrocatalytic materials for EOR over the past two decades with a focus on Pt- and Pd-based catalysts. We start with discussion on the mechanistic understanding of EOR on Pt and Pd surfaces using selected publications as examples. Consensuses from the mechanistic studies are that sufficient active surface sites to facilitate the cleavage of the C–C bond and the adsorption of water or its residue are critical for obtaining a higher electro-oxidation activity. We then show how this understanding has been applied to achieve improved performance on various Pt- and Pd-based catalysts through optimizing electronic and bifunctional effects, as well as by tuning their surface composition and structure. Finally we point out the remaining key problems in the development of anode electrocatalysts for EOR.

  2. Solid Silica-based Sulphonic Acid as an Efficient Green Catalyst for ...

    African Journals Online (AJOL)

    NJD

    Solid Silica-based Sulphonic Acid as an Efficient Green. Catalyst for the Selective Oxidation of Sulphides to. Sulphoxides using NaCIO in Aqueous Media. Ali Amoozadeh* and Firouzeh Nemati. Department of Chemistry, Faculty of Science, Semnan University, Semnan, Iran. Received 21 October 2008, revised 6 December ...

  3. Boric acid as a mild and efficient catalyst for one-pot synthesis of 1

    Indian Academy of Sciences (India)

    Abstract. An efficient green chemistry method has been developed for the synthesis of 1-amidoalkyl-2-naphthol derivatives via a one-pot three-component condensation of 2-naphthol, aldehydes and amide in the presence of boric acid as a mild catalyst.

  4. Efficient oxygen reduction reaction using ruthenium tetrakis(diaquaplatinum)octacarboxyphthalocyanine catalyst supported on MWCNT platform

    CSIR Research Space (South Africa)

    Maxakato, NW

    2011-02-01

    Full Text Available -1 Electroanalysis 2011, 23, No. 2, 325 ? 329 Efficient Oxygen Reduction Reaction Using Ruthenium Tetrakis(diaquaplatinum)Octacarboxyphthalocyanine Catalyst Supported on MWCNT Platform Nobanathi W. Maxakato,a Solomon A. Mamuru,a Kenneth I. Ozoemena*a, b a...

  5. Silica-supported ionic liquid as highly efficient catalyst for one-pot ...

    Indian Academy of Sciences (India)

    4. Conclusion. A novel multicomponent approach for the synthesis of a series of new acenaphthofuran derivatives utilizing the supported ionic liquid catalyst has been elaborated. The efficient catalysing of used ionic liquid in the synthesis of acenaphtho[1,2-b]furans led to high chemical yields as well as short reaction times.

  6. Ganoderma-Like MoS2 /NiS2 with Single Platinum Atoms Doping as an Efficient and Stable Hydrogen Evolution Reaction Catalyst.

    Science.gov (United States)

    Guan, Yongxin; Feng, Yangyang; Wan, Jing; Yang, Xiaohui; Fang, Ling; Gu, Xiao; Liu, Ruirui; Huang, Zhengyong; Li, Jian; Luo, Jun; Li, Changming; Wang, Yu

    2018-05-27

    Herein, a unique ganoderma-like MoS 2 /NiS 2 hetero-nanostructure with isolated Pt atoms anchored is reported. This novel ganoderma-like heterostructure can not only efficiently disperse and confine the few-layer MoS 2 nanosheets to fully expose the edge sites of MoS 2 , and provide more opportunity to capture the Pt atoms, but also tune the electronic structure to modify the catalytic activity. Because of the favorable dispersibility and exposed large specific surface area, single Pt atoms can be easily anchored on MoS 2 nanosheets with ultrahigh loading of 1.8 at% (the highest is 1.3 at% to date). Owing to the ganoderma-like structure and platinum atoms doping, this catalyst shows Pt-like catalytic activity for the hydrogen evolution reaction with an ultralow overpotential of 34 mV and excellent durability of only 2% increase in overpotential for 72 h under the constant current density of 10 mA cm -2 . © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-06-15

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

  8. Magnetically Separable Iron Oxide Nanoparticles: An Efficient and Reusable Catalyst for Imino Diels-Alder Reaction

    Energy Technology Data Exchange (ETDEWEB)

    Basavegowda, Nagaraj; Mishra, Kanchan; Lee, Yong Rok; Joh, Young-Gull [Yeungnam University, Gyeongsan (Korea, Republic of)

    2016-02-15

    Iron oxide nanoparticles were synthesized using Saururus chinensis (S. chinensis) leaf extract as a reducing and stabilizing agent via ultrasonication. The size, morphology, crystallinity, elemental composition, weight loss, surface chemical state, and magnetic properties of the synthesized nanoparticles were investigated. The synthe-sized nanoparticles were used as an efficient and recyclable catalyst for the synthesis of a variety of 2-methyl-4-substituted-1,2,3,4-tetrahydroquinoline derivatives by the imino Diels-Alder reaction. After the reaction, the catalyst was recovered by an external magnetic field. The recovered catalyst was then reused in a subsequent reaction under identical conditions. The recycled iron oxide nanoparticles (IONPs) were reused five times with-out any significant loss of catalytic activity.

  9. Magnetically Separable Iron Oxide Nanoparticles: An Efficient and Reusable Catalyst for Imino Diels-Alder Reaction

    International Nuclear Information System (INIS)

    Basavegowda, Nagaraj; Mishra, Kanchan; Lee, Yong Rok; Joh, Young-Gull

    2016-01-01

    Iron oxide nanoparticles were synthesized using Saururus chinensis (S. chinensis) leaf extract as a reducing and stabilizing agent via ultrasonication. The size, morphology, crystallinity, elemental composition, weight loss, surface chemical state, and magnetic properties of the synthesized nanoparticles were investigated. The synthe-sized nanoparticles were used as an efficient and recyclable catalyst for the synthesis of a variety of 2-methyl-4-substituted-1,2,3,4-tetrahydroquinoline derivatives by the imino Diels-Alder reaction. After the reaction, the catalyst was recovered by an external magnetic field. The recovered catalyst was then reused in a subsequent reaction under identical conditions. The recycled iron oxide nanoparticles (IONPs) were reused five times with-out any significant loss of catalytic activity.

  10. Pt skin coated hollow Ag-Pt bimetallic nanoparticles with high catalytic activity for oxygen reduction reaction

    Science.gov (United States)

    Fu, Tao; Huang, Jianxing; Lai, Shaobo; Zhang, Size; Fang, Jun; Zhao, Jinbao

    2017-10-01

    The catalytic activity and stability of electrocatalyst is critical for the commercialization of fuel cells, and recent reports reveal the great potential of the hollow structures with Pt skin coat for developing high-powered electrocatalysts due to their highly efficient utilization of the Pt atoms. Here, we provide a novel strategy to prepare the Pt skin coated hollow Ag-Pt structure (Ag-Pt@Pt) of ∼8 nm size at room temperature. As loaded on the graphene, the Ag-Pt@Pt exhibits a remarkable mass activity of 0.864 A/mgPt (at 0.9 V, vs. reversible hydrogen electrode (RHE)) towards oxygen reduction reaction (ORR), which is 5.30 times of the commercial Pt/C catalyst, and the Ag-Pt@Pt also shows a better stability during the ORR catalytic process. The mechanism of this significant enhancement can be attributed to the higher Pt utilization and the unique Pt on Ag-Pt surface structure, which is confirmed by the density functional theory (DFT) calculations and other characterization methods. In conclusion, this original work offers a low-cost and environment-friendly method to prepare a high active electrocatalyst with cheaper price, and this work also discloses the correlation between surface structures and ORR catalytic activity for the hollow structures with Pt skin coat, which can be instructive for designing novel advanced electrocatalysts for fuel cells.

  11. Iron doped fibrous-structured silica nanospheres as efficient catalyst for catalytic ozonation of sulfamethazine.

    Science.gov (United States)

    Bai, Zhiyong; Wang, Jianlong; Yang, Qi

    2018-04-01

    Sulfonamide antibiotics are ubiquitous pollutants in aquatic environments due to their large production and extensive application. In this paper, the iron doped fibrous-structured silica (KCC-1) nanospheres (Fe-KCC-1) was prepared, characterized, and applied as a catalyst for catalytic ozonation of sulfamethazine (SMT). The effects of ozone dosage, catalyst dosage, and initial concentration of SMT were examined. The experimental results showed that Fe-KCC-1 had large surface area (464.56 m2 g -1 ) and iron particles were well dispersed on the catalyst. The catalyst had high catalytic performance especially for the mineralization of SMT, with mineralization ratio of about 40% in a wide pH range. With addition of Fe-KCC-1, the ozone utilization increased nearly two times than single ozonation. The enhancement of SMT degradation was mainly due to the surface reaction, and the increased mineralization of SMT was due to radical mechanism. Fe-KCC-1 was an efficient catalyst for SMT degradation in catalytic ozonation system.

  12. Highly selective hydrogenation of furfural to furfuryl alcohol over Pt nanoparticles supported on g-C3N4 nanosheets catalysts in water

    OpenAIRE

    Chen, Xiufang; Zhang, Ligang; Zhang, Bo; Guo, Xingcui; Mu, Xindong

    2016-01-01

    Graphitic carbon nitride nanosheets were investigated for developing effective Pt catalyst supports for selective hydrogenation of furfural to furfuryl alcohol in water. The nanosheets with an average thickness of about 3 nm were synthesized by a simple and green method through thermal oxidation etching of bulk g-C3N4 in air. Combined with the unique feature of nitrogen richness and locally conjugated structure, the g-C3N4 nanosheets with a high surface area of 142?m2 g?1 were demonstrated to...

  13. Catalytic recombination of dissociation products with Pt/SnO2 for rare and common isotope long-life, closed-cycle CO2 lasers

    Science.gov (United States)

    Brown, Kenneth G.; Sidney, B. D.; Schryer, D. R.; Upchurch, B. T.; Miller, I. M.

    1986-01-01

    This paper reports results on recombination of pulsed CO2 laser dissociation products with Pt/SnO2 catalysts, and supporting studies in a surrogate laboratory catalyst reactor. The closed-cycle, pulsed CO2 laser has been continuously operated for one million pulses with an overall power degradation of less than 5 percent by flowing the laser gas mixture through a 2-percent Pt/SnO2 catalyst bed. In the surrogate laboratory reactor, experiments have been conducted to determine isotopic exchange with the catalyst when using rare-isotope gases. The effects of catalyst pretreatment, sample weight, composition, and temperature on catalyst efficiency have also been determined.

  14. The effect of mixed HCl–KCl competitive adsorbate on Pt adsorption and catalytic properties of Pt–Sn/Al{sub 2}O{sub 3} catalysts in propane dehydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Zangeneh, Farnaz Tahriri, E-mail: tahriri_zangeneh@yahoo.com [Department of Chemistry, Science and Research Branch, Islamic Azad University, P.O. Box 14155-4933, Tehran (Iran, Islamic Republic of); Catalyst Research Group, Petrochemical Research and Technology Company, National Petrochemical Company, P.O. Box 14358-84711, Tehran (Iran, Islamic Republic of); Taeb, Abbas [Department of Chemistry, Science and Research Branch, Islamic Azad University, P.O. Box 14155-4933, Tehran (Iran, Islamic Republic of); Gholivand, Khodayar [Department of Chemistry, Faculty of Sciences, Tarbiat Modares University, P.O. Box 14115-175, Tehran (Iran, Islamic Republic of); Sahebdelfar, Saeed [Catalyst Research Group, Petrochemical Research and Technology Company, National Petrochemical Company, P.O. Box 14358-84711, Tehran (Iran, Islamic Republic of)

    2015-12-01

    Highlights: • Impregnation is a critical step in preparation of Pt-based dehydrogenation catalysts. • A competitor ion could strongly influence the impregnation of Pt on alumina support. • The competitor type is much more effective than pH of impregnation solution. • HCl competitor can be partially replaced by KCl reducing acidic attack on support. • Adsorption parameters can be estimated by a simple equilibrium-based model. - Abstract: The effect of competitive adsorbate concentration and combination on the adsorption of H{sub 2}PtCl{sub 6} onto γ-Al{sub 2}O{sub 3} in the preparation and performance of PtSnK/γ-Al{sub 2}O{sub 3} catalyst for propane dehydrogenation was investigated. The catalysts were prepared by sequential impregnation of Sn and Pt precursors. The effect of competitor concentration on Pt adsorption was studied by using hydrochloric acid (0.1–0.3 M) and the effect of pH was studied by using KCl/HCl mixtures at constant (0.1 M) total chloride ion concentration. The catalysts were characterized by nitrogen adsorption/desorption, XRD, XRF, SEM and CO chemisorption. The catalytic performance tests were carried out in a fixed-bed quartz reactor under kinetic controlled condition for proper catalyst screening. It was found that the corrosive competitor HCl could be partially substituted with KCl without appreciable impact on catalyst performance with the advantage of lower acid attack on the support and reduced leaching of the deposited tin. A model based on initial concentration and uptake of the adsorbates was developed to obtain the adsorption parameters. Values of 890 μmol/g and 600 lit/mol were obtained for adsorption site concentration of the tin-impregnated support and equilibrium constant for Pt adsorption, respectively, for HCl concentration range of 0.1–0.3 M.

  15. Efficient filtration system for paraffin-catalyst slurry separation

    Directory of Open Access Journals (Sweden)

    Khodagholi Mohammad Ali

    2013-01-01

    Full Text Available The filtration efficiency for separating liquid paraffin (or water from a slurry consisting of 25 weight% spherical alumina in a Slurry Bubble Column Reactor (SBCR comprised of a cylindrical tube of 10 cm diameter and 150 cm length was studied. Various differential pressures (ΔP were applied to two separate tubular sintered metal stainless steel filter elements with nominal pore size of 4 and 16μm. The experimental results disclosed that the rate of filtrations increased on applying higher differential pressure to the filter element. Albeit this phenomenon is limited to moderate ΔPs and for ΔP more than 1 bar is neither harmful nor helpful. The highest filtration rates at ΔPs higher than 1 bar were 170 and 248 ml/minute for 4 and 16μm respectively. Using water as the liquid in slurry the rate of filtration enhanced to 4 folds, and this issue reveals impact of viscosity on filtration efficiency clearly. In all situations, the total amount of particles present in the filtrate part never exceeded a few parts per million (ppm. The statistical analysis of the SEM image of the filtrate indicated that by applying higher pressure difference to the filter element the frequency percent of larger particle size increases. The operation of filter cake removing was performed with back flashing of 300 ml of clean liquid with pressures of 3-5 bar of N2 gas.

  16. Hydrogen evolution from aqueous-phase photocatalytic reforming of ethylene glycol over Pt/TiO{sub 2} catalysts: Role of Pt and product distribution

    Energy Technology Data Exchange (ETDEWEB)

    Li, Fuying [State Key Laboratory of Photocatalysis on Energy and Environment, Research Institute of Photocatalysis, Fuzhou University, Fuzhou 350002 (China); College of Resources and Chemical Engineering, Sanming University, Sanming 365004 (China); Gu, Quan [Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shanxi Normal University, Xi’an 710062 (China); Niu, Yu [College of Resources and Chemical Engineering, Sanming University, Sanming 365004 (China); School of Chemical Engineering, Fuzhou University, Fuzhou 350116 (China); Wang, Renzhang [College of Resources and Chemical Engineering, Sanming University, Sanming 365004 (China); Tong, Yuecong; Zhu, Shuying; Zhang, Hualei [State Key Laboratory of Photocatalysis on Energy and Environment, Research Institute of Photocatalysis, Fuzhou University, Fuzhou 350002 (China); Zhang, Zizhong, E-mail: z.zhang@fzu.edu.cn [State Key Laboratory of Photocatalysis on Energy and Environment, Research Institute of Photocatalysis, Fuzhou University, Fuzhou 350002 (China); Wang, Xuxu [State Key Laboratory of Photocatalysis on Energy and Environment, Research Institute of Photocatalysis, Fuzhou University, Fuzhou 350002 (China)

    2017-01-01

    Highlights: • Photocatalytic EG reforming generates many hydrocarbons besides H{sub 2}, CO{sub 2} and CO. • Pt loading greatly improves the photocatalytic activity of TiO{sub 2} for EG reforming. • Half amount of the produced H{sub 2} over Pt/TiO{sub 2} originates from EG reforming. - Abstract: Pt nanoparticles were loaded on anatase TiO{sub 2} by the photodeposition method to investigate their photocatalytic activity for H{sub 2} evolution in an aqueous solution containing a certain amount of ethylene glycol (EG) as the sacrificial agent. The surface properties and chemical states of the Pt/TiO{sub 2} sample were characterized by X-ray powder diffraction analysis, Brunauer–Emmett–Teller surface area analysis, transmission electron microscopy, X-ray photoelectron spectroscopy, electron paramagnetic resonance, and electrochemical resistance. The aqueous-phase photocatalytic EG reforming using Pt/TiO{sub 2} and anatase TiO{sub 2} generated not only H{sub 2} and CO{sub 2}, but also CO, CH{sub 4}, C{sub 2}H{sub 6}, and C{sub 2}H{sub 4}. Moreover, the amount of formate and acetate complexes in the solution increased gradually. The EG adsorption and gas-phase intermediates during photocatalytic reaction processes were investigated by the in situ FTIR spectrum. Finally, the photocatalytic EG reforming reaction mechanism was elucidated. This helped to better understand the role of a sacrificial agent in a photocatalytic hydrogen production.

  17. Sn surface-enriched Pt-Sn bimetallic nanoparticles as a selective and stable catalyst for propane dehydrogenation

    KAUST Repository

    Zhu, Haibo; Anjum, Dalaver H.; Wang, Qingxiao; Abou-Hamad, Edy; Emsley, Lyndon; Dong, Hailin; Laveille, Paco; Li, Lidong; Samal, Akshaya Kumar; Basset, Jean-Marie

    2014-01-01

    Sn(n-C4H9) are chemically linked to the surface of Pt NPs to produce, in fine, after removal of most of the n-butyl fragment, bimetallic Pt-Sn nanoparticles. The Sn(n-CH2CH2CH2CH3) groups remaining at the surface are believed to stabilize the as

  18. Morphological features of electrodeposited Pt nanoparticles and its application as anode catalysts in polymer electrolyte formic acid fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Jeon, Hongrae; Joo, Jiyong; Kwon, Youngkook [Electrochemical Reaction and Technology Laboratory (ERTL), Department of Environmental Science and Engineering, GIST, Gwangju 500-712 (Korea); Uhm, Sunghyun [Ertl Center for Electrochemistry and Catalysis, GIST, Gwangju 500-712 (Korea); Lee, Jaeyoung [Electrochemical Reaction and Technology Laboratory (ERTL), Department of Environmental Science and Engineering, GIST, Gwangju 500-712 (Korea); Ertl Center for Electrochemistry and Catalysis, GIST, Gwangju 500-712 (Korea)

    2010-09-15

    Electrodeposited Pt nanoparticles on carbon substrate show various morphologies depending on the applied potentials. Dendritic, pyramidal, cauliflower-like, and hemi-spherical morphologies of Pt are formed at potential ranges between -0.2 and 0.3 V (vs. Ag/AgCl) and its particle sizes are distributed from 8 to 26 nm. Dendritic bulky particles over 20 nm are formed at an applied potential of -0.2 V, while low deposition potential of 0.2 V causes dense hemi-spherical structure of Pt less than 10 nm. The influence of different Pt shapes on an electrocatalytic oxidation of formic acid is represented. Consequently, homogeneous distribution of Pt nanoparticles with average particle of ca. 14 nm on carbon paper results in a high surface to volume ratio and the better power performance in a fuel cell application. (author)

  19. Efficient switching of 3-terminal magnetic tunnel junctions by the giant spin Hall effect of Pt85Hf15 alloy

    Science.gov (United States)

    Nguyen, Minh-Hai; Shi, Shengjie; Rowlands, Graham E.; Aradhya, Sriharsha V.; Jermain, Colin L.; Ralph, D. C.; Buhrman, R. A.

    2018-02-01

    Recent research has indicated that introducing impurities that increase the resistivity of Pt can enhance the efficiency of the spin Hall torque it generates. Here, we directly demonstrate the usefulness of this strategy by fabricating prototype 3-terminal in-plane-magnetized magnetic tunnel junctions that utilize the spin Hall torque from a Pt85Hf15 alloy and measuring the critical currents for switching. We find that Pt85Hf15 reduces the switching current densities compared to pure Pt by approximately a factor of 2 for both quasi-static ramped current biases and nanosecond-scale current pulses, thereby proving the feasibility of this approach in assisting the development of efficient embedded magnetic memory technologies.

  20. Effect of cationic molecules on the oxygen reduction reaction on fuel cell grade Pt/C (20 wt%) catalyst in potassium hydroxide (aq, 1 mol dm(-3)).

    Science.gov (United States)

    Ong, Ai Lien; Inglis, Kenneth K; Whelligan, Daniel K; Murphy, Sam; Varcoe, John R

    2015-05-14

    This study investigates the effect of 1 mmol dm(-3) concentrations of a selection of small cationic molecules on the performance of a fuel cell grade oxygen reduction reaction (ORR) catalyst (Johnson Matthey HiSPEC 3000, 20 mass% Pt/C) in aqueous KOH (1 mol dm(-3)). The cationic molecules studied include quaternary ammonium (including those based on bicyclic systems) and imidazolium types as well as a phosphonium example: these serve as fully solubilised models for the commonly encountered head-groups in alkaline anion-exchange membranes (AAEM) and anion-exchange ionomers (AEI) that are being developed for application in alkaline polymer electrolyte fuel cells (APEFCs), batteries and electrolysers. Both cyclic and hydrodynamic linear sweep rotating disk electrode voltammetry techniques were used. The resulting voltammograms and subsequently derived data (e.g. apparent electrochemical active surface areas, Tafel plots, and number of [reduction] electrons transferred per O2) were compared. The results show that the imidazolium examples produced the highest level of interference towards the ORR on the Pt/C catalyst under the experimental conditions used.

  1. Synthesis and physicochemical properties of Zr-MCM-41 mesoporous molecular sieves and Pt/H3PW12O40/Zr-MCM-41 catalysts

    International Nuclear Information System (INIS)

    Chen, L.F.; Wang, J.A.; Norena, L.E.; Aguilar, J.; Navarrete, J.; Salas, P.; Montoya, J.A.; Del Angel, P.

    2007-01-01

    For the first time, modifications of the surface and framework of Si-MCM-41 by depositing a heteropolyacid on the surface and by introducing foreign Zr 4+ ions into the framework are investigated. The Zr-modified Si-MCM-41 mesoporous materials (hereafter referred as WSZn, n=Si/Zr=25, 15, 8, 4) were synthesized through a surfactant-templated preparation approach, using low-cost fumed silica as the Si precursor. After impregnation with 25 wt% of H 3 PW 12 O 40 , the surface Broensted acidity of the Pt/H 3 PW 12 O 40 /WSZn catalysts was greatly enhanced by 2-10 times relative to the bare WSZn support. Two kinds of supported heteropolyacids were formed: (i) bulk-like heteropolyacid crystals with unchanged Keggin structures, and (ii) highly dispersed heteropolyacid with distorted Keggin units. The formation of various kinds of heteropolyacid structures is closely related to the interaction between the heteropolyanions and the hydroxyl groups in the host support. - Graphical abstract: Modifications of the surface and framework of Si-MCM-41 by depositing a heteropolyacid on the surface and by introducing foreign Zr 4+ ions into the framework are investigated. Broensted acidity of the Pt/H 3 PW 12 O 40 /Zr-MCM-41 catalysts was greatly enhanced by 2-10 times relative to the bare Zr-MCM-41 support

  2. Zirconyl (IV Nitrate as Efficient and Reusable Solid Lewis Acid Catalyst for the Synthesis of Benzimidazole Derivatives

    Directory of Open Access Journals (Sweden)

    Pratapsinha B. Gorepatil

    2013-01-01

    Full Text Available The present paper introduces a simple and efficient method for the synthesis of substituted benzimidazoles by heterocyclization of different o-phenylenediamines and substituted aromatic carboxylic acid/aldehyde in the presence of zirconyl nitrate as catalyst in ethanol under reflux, which produced excellent yield of corresponding benzimidazoles in a short reaction time with reusability of catalyst.

  3. Nano-Ticl 4 .SiO 2 : a Versatile and Efficient Catalyst for Synthesis of ...

    African Journals Online (AJOL)

    Nano-TiCl4.SiO2 has been found to be an extremely efficient catalyst for the preparation of 3,4-dihydropyrimidinones/thiones via three-component reactions of an aldehyde, β-ketoester or β-diketone and urea or thiourea under mild conditions. Nano-TiCl4.SiO2 as a solid Lewis acid has been synthesized by reaction of ...

  4. XRD (X-Ray Diffraction) and nitrogen adsorption characterization of Ni-Pt/mordenite catalysts; Caracterizacao por EDX (Espectrometria de Raios-X), DRX (Difracao de Raios-X) e adsorcao de nitrogenio de catalisadores Ni/Pt/mordenita visando sua aplicacao na isomerizacao de n-hexano

    Energy Technology Data Exchange (ETDEWEB)

    Martins, Geovana do Socorro V.; Sousa, Bianca V.; Rodrigues, Meiry Glaucia F. [Universidade Federal de Campina Grande (UFCG), PB (Brazil)

    2008-07-01

    The search for molecules of high octane arose great interest in the isomerization processes. Catalysts to the zeolite base have been wide developed for the n-paraffins isomerization. In this work, bimetallic bifunctional catalysts supported on Mordenite zeolite were prepared samples containing 60Pt40Ni (wt.%) metal (Pt). The catalysts were obtained by competitive ion exchange using aqueous solutions of [Pt(NH{sub 3}){sub 4}]Cl{sub 2} and Ni(NH{sub 3}){sub 6}]Cl{sub 2} complexes. The EDS characterization analyses showed incorporation of the nickel and platinum mordenite zeolite. The diffractograms showed competitive ion exchange and calcination processes did not provoke appreciable changes in the zeolitic support framework. The peaks attributed to nickel and platinum oxides was possible to observe in the bimetallic catalysts 60Ni40Pt/MOR. The results of the N{sub 2} physical adsorption of the 60Ni40Pt/MOR showed that it did not have modification in the superficial area of the catalysts. (author)

  5. Direct synthesis of bimetallic PtCo mesoporous nanospheres as efficient bifunctional electrocatalysts for both oxygen reduction reaction and methanol oxidation reaction

    Science.gov (United States)

    Wang, Hongjing; Yu, Hongjie; Li, Yinghao; Yin, Shuli; Xue, Hairong; Li, Xiaonian; Xu, You; Wang, Liang

    2018-04-01

    The engineering of electrocatalysts with high performance for cathodic and/or anodic catalytic reactions is of great urgency for the development of direct methanol fuel cells. Pt-based bimetallic alloys have recently received considerable attention in the field of fuel cells because of their superior catalytic performance towards both fuel molecule electro-oxidation and oxygen reduction. In this work, bimetallic PtCo mesoporous nanospheres (PtCo MNs) with uniform size and morphology have been prepared by a one-step method with a high yield. The as-made PtCo MNs show superior catalytic activities for both oxygen reduction reaction and methanol oxidation reaction relative to Pt MNs and commercial Pt/C catalyst, attributed to their mesoporous structure and bimetallic composition.

  6. Size and morphology controlled NiSe nanoparticles as efficient catalyst for the reduction reactions

    Energy Technology Data Exchange (ETDEWEB)

    Subbarao, Udumula; Marakatti, Vijaykumar S. [New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India); Amshumali, Mungalimane K. [New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India); Department of Chemistry and Industrial Chemistry, Vijayanagara Sri Krishnadevaraya University, Jnanasagara Campus, Cantonment, Bellary 583105 (India); Loukya, B. [International Center for Materials Science, Jakkur P.O., Bangalore 560064 (India); Singh, Dheeraj Kumar [Chemistry & Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India); Datta, Ranjan [International Center for Materials Science, Jakkur P.O., Bangalore 560064 (India); Peter, Sebastian C., E-mail: sebastiancp@jncasr.ac.in [New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India)

    2016-12-15

    Facile and efficient ball milling and polyol methods were employed for the synthesis of nickel selenide (NiSe) nanoparticle. The particle size of the NiSe nanoparticle has been controlled mechanically by varying the ball size in the milling process. The role of the surfactants in the formation of various morphologies was studied. The compounds were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray energy dispersive spectroscopy (EDS). The efficiency of the NiSe nanoparticle as a catalyst was tested for the reduction of para-nitroaniline (PNA) to para-phenyldiamine (PPD) and para-nitrophenol (PNP) to para-aminophenol (PAP) using NaBH{sub 4} as the reducing agent. Particle size, morphology and the presence of surfactant played a crucial role in the reduction process. - Graphical abstract: NiSe nanoparticles in different size and morphology were synthesized using facile ball milling and polyol methods. Particle size, morphology and the presence of surfactant in these materials played a crucial role in the hydrogenation of PNA and PNP. - Highlights: • NiSe nanoparticles synthesized using ball milling and solution phase methods. • NiSe nanoparticle is an efficient catalyst for the reduction of PNA and PNP. • NiSe is found to be better than the best reported noble metal catalysts.

  7. Size and morphology controlled NiSe nanoparticles as efficient catalyst for the reduction reactions

    International Nuclear Information System (INIS)

    Subbarao, Udumula; Marakatti, Vijaykumar S.; Amshumali, Mungalimane K.; Loukya, B.; Singh, Dheeraj Kumar; Datta, Ranjan; Peter, Sebastian C.

    2016-01-01

    Facile and efficient ball milling and polyol methods were employed for the synthesis of nickel selenide (NiSe) nanoparticle. The particle size of the NiSe nanoparticle has been controlled mechanically by varying the ball size in the milling process. The role of the surfactants in the formation of various morphologies was studied. The compounds were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray energy dispersive spectroscopy (EDS). The efficiency of the NiSe nanoparticle as a catalyst was tested for the reduction of para-nitroaniline (PNA) to para-phenyldiamine (PPD) and para-nitrophenol (PNP) to para-aminophenol (PAP) using NaBH 4 as the reducing agent. Particle size, morphology and the presence of surfactant played a crucial role in the reduction process. - Graphical abstract: NiSe nanoparticles in different size and morphology were synthesized using facile ball milling and polyol methods. Particle size, morphology and the presence of surfactant in these materials played a crucial role in the hydrogenation of PNA and PNP. - Highlights: • NiSe nanoparticles synthesized using ball milling and solution phase methods. • NiSe nanoparticle is an efficient catalyst for the reduction of PNA and PNP. • NiSe is found to be better than the best reported noble metal catalysts.

  8. Phosphorene Co-catalyst Advancing Highly Efficient Visible-Light Photocatalytic Hydrogen Production.

    Science.gov (United States)

    Ran, Jingrun; Zhu, Bicheng; Qiao, Shi-Zhang

    2017-08-21

    Transitional metals are widely used as co-catalysts boosting photocatalytic H 2 production. However, metal-based co-catalysts suffer from high cost, limited abundance and detrimental environment impact. To date, metal-free co-catalyst is rarely reported. Here we for the first time utilized density functional calculations to guide the application of phosphorene as a high-efficiency metal-free co-catalyst for CdS, Zn 0.8 Cd 0.2 S or ZnS. Particularly, phosphorene modified CdS shows a high apparent quantum yield of 34.7 % at 420 nm. This outstanding activity arises from the strong electronic coupling between phosphorene and CdS, as well as the favorable band structure, high charge mobility and massive active sites of phosphorene, supported by computations and advanced characterizations, for example, synchrotron-based X-ray absorption near edge spectroscopy. This work brings new opportunities to prepare highly-active, cheap and green photocatalysts. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. 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.

  10. Vertically aligned carbon nanotubes/carbon fiber paper composite to support Pt nanoparticles for direct methanol fuel cell application

    Science.gov (United States)

    Zhang, Jing; Yi, Xi-bin; Liu, Shuo; Fan, Hui-Li; Ju, Wei; Wang, Qi-Chun; Ma, Jie

    2017-03-01

    Vertically aligned carbon nanotubes (VACNTs) grown on carbon fiber paper (CFP) by plasma enhanced chemical vapor deposition is introduced as a catalyst support material for direct methanol fuel cells (DMFCs). Well dispersed Pt nanoparticles on VACNTs surface are prepared by impregnation-reduction method. The VACNTs on CFP possess well-maintained alignment, large surface area and good electrical conductivity, which leading to the formation of Pt particles with a smaller size and enhance the Pt utilization rate. The structure and nature of resulting Pt/VACNTs/CFP catalysts for methanol oxidation are investigated by transmission electron microscopy (TEM), X-ray diffraction (XRD) and scanning electron microscope (SEM). With the aid of VACNTs, well-dispersed Pt catalysts enable the reversibly rapid redox kinetic since electron transport efficiently passes through a one-dimensional pathway, which leads to enhance the catalytic activity and Pt utilization rate. Compared with the Pt/XC-72/CFP electrode, the electrochemical measurements results display that the Pt/VACNTs/CFP catalyst shows much higher electrocatalytic activity and better stability for methanol oxidation. In addition, the oxidation current from 200 to 1200 s decayed more slowly for the Pt/VACNTs/CFP than that of the Pt/XC-72/CFP catalysts, indicating less accumulation of adsorbed CO species. All those results imply that the Pt/VACNTs/CFP has a great potential for applications in DMFCs.

  11. Electroplating sludge derived zinc-ferrite catalyst for the efficient photo-Fenton degradation of dye.

    Science.gov (United States)

    Cao, Zhenbang; Zhang, Jia; Zhou, Jizhi; Ruan, Xiuxiu; Chen, Dan; Liu, Jianyong; Liu, Qiang; Qian, Guangren

    2017-05-15

    A zinc-dominant ferrite catalyst for efficient degradation of organic dye was prepared by the calcination of electroplating sludge (ES). Characterizations indicated that zinc ferrite (ZnFe 2 O 4 ) coexisted with Fe 2 O 3 structure was the predominant phase in the calcined electroplating sludge (CES). CES displayed a high decolorization ratio (88.3%) of methylene blue (MB) in the presence of H 2 O 2 combined with UV irradiation. The high efficiency could be ascribed to the photocatalytic process induced by ZnFe 2 O 4 and the photo-Fenton dye degradation by ferrous content, and a small amount of Al and Mg in the sludge might also contribute to the catalysis. Moreover, the degradation capability of dye by CES was supported by the synthetic ZnFe 2 O 4 with different Zn to Fe molar ratio (n(Zn): n(Fe)), as 84.81%-86.83% of dye was removed with n(Zn): n(Fe) ranged from 1:0.5 to 1:3. All synthetic ferrite samples in the simulation achieved adjacent equilibrium decolorization ratio, the flexible proportioning of divalent metal ions (M 2+ ) to trivalent metal ions (M 3+ ) applied in the synthesis indicated that the catalyst has a high availability. Therefore, an efficacious catalyst for the degradation of dye can potentially be derived from heavy metal-containing ES, it's a novel approach for the reutilization of ES. Copyright © 2016 Elsevier Ltd. All rights reserved.

  12. Kinetics of catalytic reforming with Pt-Sn catalyst; Modelisation cinetique du reformage catalytique sur catalyseur Pt-Sn/Al{sub 2}O{sub 3}

    Energy Technology Data Exchange (ETDEWEB)

    Cochegrue, H.

    2001-04-01

    Catalytic Reforming is one of the key processes for petrol refining as it produces gasoline with a high octane number and it is a main source of hydrogen. Refiners are asking for more accurate models in order to optimise their plants. An innovative methodology called 'Single Events' is very different from the classical empirical models because it takes into account the various reaction intermediates and reaction pathways. Some hypotheses based on the relative stability of the carbo-cations allow to get a small number of parameters, which are independent of the composition of the feedstock used. The main target of this work was to apply this methodology to the Catalytic Reforming. The single event network had to be first reduced to a late lumped reaction scheme, which incorporates the detailed knowledge of the elementary network while the intermediates and the reaction pathways are reduced: it can be applied now to naphtha feedstock, although the detailed composition is not yet well known. A pilot unit of Catalytic Reforming, which is representative of the industrial processes, was first designed for the kinetic experiments. Experiments with technical heptane were conducted with a fresh catalyst, which was cocked first, and with a used catalyst from a refinery plant. This latter was difficult to use because of its fast deactivation. However, the results obtained allowed to study the influence of the experimental parameters and of the poisoning by iron, and to estimate some of the main kinetic parameters of the model. (author)

  13. Copper oxide as efficient catalyst for oxidative dehydrogenation of alcohols with air

    DEFF Research Database (Denmark)

    Poreddy, Raju; Engelbrekt, Christian; Riisager, Anders

    2015-01-01

    The oxidative dehydrogenation of alcohols to carbonyl compounds was studied using CuO nanoparticle catalysts prepared by solution synthesis in buffered media. CuO nanoparticles synthesized in N-cyclohexyl- 3-aminopropanesulfonic acid buffer showed high catalytic activity for the oxidation...... of benzylic, alicyclic and unsaturated alcohols to their corresponding carbonyl compounds with excellent selectivities. The observed trend in activity for conversion of substituted alcohols suggested a β-H elimination step to be involved, thus enabling a possible reaction mechanism for oxidative...... dehydrogenation of benzyl alcohols to be proposed. The use of CuO as an inexpensive and efficient heterogeneous catalyst under aerobic conditions provides a new noble metal-free and green reaction protocol for carbonyl compound synthesis....

  14. Core-shell structural nanodiamond@TiN supported Pt nanoparticles as a highly efficient and stable electrocatalyst for direct methanol fuel cells

    International Nuclear Information System (INIS)

    Zhao, Yuling; Wang, Yanhui; Dong, Liang; Zhang, Yan; Huang, Junjie; Zang, Jianbing; Lu, Jing; Xu, Xipeng

    2014-01-01

    Highlights: • Core-shell structural nanodiamond@TiN was used as a novel support for Pt catalysts. • The ND@TiN support possessed a high electrochemical stability than carbon black. • The Pt/ND@TiN showed a higher catalytic activity for MOR and ORR than the Pt/C. • The Pt/ND@TiN demonstrated a much better durability compared with the Pt/C. - Abstract: A novel core-shell support material was designed with nanodiamond (ND) as core possessed excellent stability and TiN as shell improved the conductivity of support. The nano-TiN shell was decorated on the surface of ND by annealing TiO 2 in nitrogen atmosphere, and the obtained ND@TiN was employed to support Pt nanoparticles (NPs). The ND@TiN support and Pt/ND@TiN electrocatalyst were characterized by X-ray diffraction and transmission electron microscopy. ND particles were coated uniformly by the TiN layer and Pt NPs with a mean size of 4.2 nm were highly dispersed on the surface of ND@TiN. The electrochemical results confirmed that the ND@TiN support possessed a much more stability than the carbon black and exhibited a bigger background current density than the ND. The Pt/ND@TiN catalyst showed higher catalytic activity and better stability in methanol oxidation and oxygen reduction reactions compared with the Pt/C and Pt/ND

  15. Design of bimetal catalysts Pt-Ni/CeO{sub 2}-1D for generation of H{sub 2} by the reforming reaction of methanol; Diseno de catalizadores bimetalicos Pt-Ni/CeO{sub 2}-1D para generacion de H{sub 2} mediante la reaccion de reformado de metanol

    Energy Technology Data Exchange (ETDEWEB)

    Sarmiento F, I.

    2016-07-01

    CeO{sub 2} nano rods were synthesized by hydrothermal method and were used as support for preparing catalysts bimetallic Pt Ni / CeO{sub 2}-1D. The catalysts were prepared by classical impregnation by the conventional wet method. The prepared catalysts are Pt (0.5 %) - Ni (5 %) / CeO{sub 2} and Pt (0.5 %) - Ni (15 %) / CeO{sub 2}, which were characterized by different physico-chemical techniques: Bet, Sem, TPR and XRD, that were evaluated in the Auto thermal Steam reforming of Methanol for H{sub 2} production. The Bet surface area results, show that the surface area of the catalysts decreases as the nominal load of Ni in the catalyst, increases. Sem shows, that the catalyst support (CeO{sub 2}-1D) and the bimetallic catalysts are conformed by nano rods. By XRD were identified the crystalline phases present, in the catalytic material: cerianite distinctive phase of cerium oxide and metallic Ni; however it was not possible to observe diffraction peaks of Platinum using this technique. The temperature-programmed reduction (TPR) analysis allowed to obtain the reduction profiles, of the different species present on the catalysts. The catalytic activity tests carried out, showed that the catalysts total 100% methanol conversion is achieved at 300 degrees Celsius, making them excellent, to be used in reactions at low temperature conditions. Selectivity towards H{sub 2}, is very similar in both catalysts, and it reaches a 50% yield per mole of methanol fed stoichiometrically. (Author)

  16. Modification of the properties of Pt-Al/sub 2/O/sub 3/ catalysts by hydrogen at high temperatures

    Energy Technology Data Exchange (ETDEWEB)

    Menon, P.G.; Froment, G.F.

    1979-08-01

    Pulse reactor studies were performed on the hydrogenolysis of n-pentane and n-hexane at 400/sup 0/C on two commercial reforming catalysts that contained 0.6 and 0.75% platinum on alumina, respectively, and which were calcined in air at 500/sup 0/C, followed by hydrogen-reduction at 400/sup 0/-600/sup 0/C. On catalysts reduced at 400/sup 0/C, hydrogenolysis was the main reaction; with increasing reducing temperature, hydrogenolysis was suppressed and isomerization selectivity increased; at 550/sup 0/C pretreatment temperature, hydrogenolysis was near zero. This selective catalyst deactivation was reversed by oxidizing the catalyst in air at 500/sup 0/C in a similar manner as previously found for sulfided and chlorided catalysts. Temperature-programed desorption of hydrogen adsorbed at 20/sup 0/-600/sup 0/C revealed that the higher the adsorption temperature, the higher the temperature of the hydrogen desorption peaks: the hydrogen adsorbed below 400/sup 0/C desorbed mainly at 50/sup 0/-300/sup 0/C, but the hydrogen adsorbed at higher temperatures desorbed at 300/sup 0/-500/sup 0/C. Apparently, two types of hydrogen adsorb in the two temperature regions, of which the more strongly adsorbed type inhibits hydrogenolysis but not isomerization.

  17. Fabrication 3 dimensional Pt catalysts via Na2Ti3O7 nanowires for methanol and ethanol electrooxidation

    Energy Technology Data Exchange (ETDEWEB)

    He, X.; Hu, C. [Chongqing Univ., Chongqing (China). Dept. of Applied Physics

    2010-07-01

    This paper reported on a study in which platinum (Pt) nanoparticles deposited on Na{sub 2}Ti{sub 3}O{sub 7} nanowires were used for the electrooxidation of methanol and ethanol in acidic and alkaline media. The Na{sub 2}Ti{sub 3}O{sub 7} nanowires were used as 3D frames for loading Pt nanoparticles. The synthesized samples were characterized by X-ray diffraction, field emission scanning electron microscopy and energy dispersive X-ray spectroscopy. The analysis revealed that Pt nanoparticles ar