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Sample records for raney ni catalyst

  1. Hydrogenolysis of 2-tosyloxy-1,3-propanediol into 1,3-propanediol over Raney Ni catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Zhi, Zheng; Jianli, Wang; Zhen, Lu; Min, Luo; Miao, Zhang; Lixin, Xu; Jianbing [Zhejiang Province Key Laboratory of Biofuel, The State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou (China)

    2013-03-15

    2-Tosyloxy-1,3-propanediol (TPD), a potential precursor for 1,3-propanediol (1,3-PD) production, is produced by the tosylation of glycerol with the help of protecting group techniques. In this work, the hydrogenolysis of TPD into 1,3-PD over Raney Ni catalyst is discussed at different reaction parameters to optimize the reaction conditions for selective formation of 1,3-PD. The mechanisms of the hydrogenolysis of TPD and the side reactions were also confirmed by gas chromatography-mass spectrometry (GC-MS) technique (author)

  2. Hydrogen production via methane decomposition on Raney-type catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Figueiredo, J.L.; Orfao, J.J.M.; Cunha, A.F. [Laboratorio de Catalise e Materiais, Laboratorio Associado LSRE/LCM, Departamento de Engenharia Quimica, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, 4200-465 Porto (Portugal)

    2010-09-15

    The catalytic decomposition of methane into hydrogen and carbon was studied on La{sub 2}O{sub 3} doped Ni and Ni-Cu Raney-type catalysts. The activity and stability of the catalysts were assessed by comparing the experimental conversions with the calculated equilibrium conversions for each set of experimental conditions, and the maximum conversions with the conversions at the end of (at least) 5 h tests, respectively. Improved stability of La{sub 2}O{sub 3} doped catalysts was ascribed to an electronic promotion effect. There is an optimum load of the promoter, which provides for extended periods of stable catalyst operation. The carbon deposits consist of carbon nanofibers and multiwall carbon nanotubes. The La{sub 2}O{sub 3} doped Ni-Cu Raney-type catalysts presented in this work are remarkably efficient for the production of hydrogen by methane decomposition. (author)

  3. TOTAL HYDROGENATION OF BIOMASS-DERIVED FURFURAL OVER RANEY NICKEL-CLAY NANOCOMPOSITE CATALYSTS

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    Rodiansono Rodiansono

    2013-08-01

    Full Text Available Inexpensive Raney Ni-clay composite (R-Ni/clay catalysts exhibited excellent activity and reusability in the total hydrogenation of biomass-derived furfural into tetrahydrofurfuryl alcohol under mild conditions. For the Raney Ni-bentonite (R-Ni/BNT catalysts, the complete reaction was achieved at 393 K, 180 min giving almost 99% yield of tetrahydrofurfuryl alcohol. The R-Ni/BNT catalyst was found to be reusable without any significant loss of activity and selectivity for at least six consecutive runs.

  4. Methane decomposition on Fe-Cu Raney-type catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Cunha, A.F.; Orfao, J.J.M.; Figueiredo, J.L. [Laboratorio de Catalise e Materiais, Laboratorio Associado LSRE/LCM, Departamento de Engenharia Quimica, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, 4200-465 Porto (Portugal)

    2009-10-15

    The decomposition of methane into hydrogen and carbon was studied on Fe-Cu catalysts of Raney-type. The activity of the catalysts was assessed by comparing the experimental conversions with the calculated equilibrium conversions for each set of experimental conditions. The stability of the catalysts was assessed by comparing the maximum conversions with the conversions at the end of 5-hour tests. The carbon deposits obtained consist mostly of carbon nanofibers. Good results were obtained when the Fe-Cu Raney-type systems were thermally treated in situ at 600 C, as a result of incipient alloy formation. These catalysts showed higher stability than the monometallic Raney-Fe catalysts. (author)

  5. Polymer-Supported Raney Nickel Catalysts for Sustainable Reduction Reactions

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    Haibin Jiang

    2016-06-01

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

  6. Novel methods of stabilization of Raney-Nickel catalyst for fuel-cell electrodes

    Energy Technology Data Exchange (ETDEWEB)

    Al-Saleh, M.A.; Sleem-Ur-Rahman; Kareemuddin, S.M.M.J.; Al-Zakri, A.S. [Dept. of Chemical Engineering, King Fahd Univ. of Petroleum and Minerals, Dhahran (Saudi Arabia)

    1998-04-21

    Two new methods of stabilizing Raney-Nickel (Raney-Ni) catalyst for making fuel-cell anodes were studied. In the first method, the catalyst was oxidized with aqueous H{sub 2}O{sub 2} solution, while in the second, oxygen/air (O{sub 2}/air) was used in a slurry reactor. Effects of different concentrations of H{sub 2}O{sub 2} (5-25 wt.%) and different pressures (10-20 psig) of gas were investigated. The stabilized catalyst was characterized using BET surface area, scanning electron microscopy (SEM) and X-ray diffraction (XRD). The catalyst was used in fuel-cell anodes and the electrochemical performance was determined in an alkaline half-cell. The results were compared with electrodes prepared using conventionally stabilized catalysts. The hydrogen peroxide-treated catalyst has higher BET surface area and produces electrodes with lower polarization. In addition to this, H{sub 2}O{sub 2} treatment is convenient, fast and needs simple equipment which involves no instrumentation. Use of oxygen in a slurry reactor to stabilize the catalyst is also convenient but electrode performance is relatively poor. (orig.)

  7. Raney copper catalysts for the water-gas shift reaction - II. Initial catalyst optimisation

    CSIR Research Space (South Africa)

    Mellor, JR

    1997-12-23

    Full Text Available -Zn-A1 catalyst. During the controlled passivation Table 2 Crystalline phase of alloys B, C and D and their product Raney copper catalysts before and after reaction Alloy Precursor alloy phases Cat. phases before reaction a Cat. phases after reaction a... L; dry gas composition=10% CO/90% N2; CO : H20=I : 22.5; catalyst volume=2i0.1 ml): (O)=Cat. A Cu(69.3)Zn(6.9)Al( 19.5); (~)=cat. B Cu(73.6)Zn(10.9)AI(14.8); (W1)=cat. C Cu(72.4)Zn(13.3)Al(12.9); ({))=cat. D Cu(61.5)Zn(15.1)AI(19.1). It can...

  8. Preparation of Raney-Ni gas diffusion electrode by filtration method for alkaline fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Sleem-Ur-Rahman; Al-Saleh, M.A.; Al-Zakri, A.S.; Gultekin, S. [King Fahd Univ. of Petroleum and Minerals, Dhahran (Saudi Arabia). Dept. of Chemical Emgineering

    1997-02-01

    A novel filtration method for preparation of gas diffusion electrodes for fuel cells is proposed. This method, which is a modification of the conventional dry method, has the merits of both wet and dry techniques. The electrode performance is improved due to better structure, controlled hydrophobicity and less compaction. To compare the effectiveness of the method, Raney-Ni/PTFE anodes for use in a KOH fuel cell were made. Their electrochemical performance was compared with similar electrodes produced by the dry method by other research groups, under the same conditions. The filtration method electrodes performed better between temperatures of 25{sup o}C and 75{sup o}C. The electrode exhibited no significant degradation of activity in the first 180 h at 100 mAcm{sup -2} anodic load. (author)

  9. Synthesis of liquid menthol by hydrogenation of dementholized peppermint oil over Ni catalysts

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    Debora L. Manuale

    2010-01-01

    Full Text Available Hydrogenation of (--menthone and (+-isomenthone was studied at 2.7 MPa and 100 ºC. The objective was to produce a liquid menthol mixture rich in (--menthol from dementholized peppermint oil. Ni-based catalysts were tested and compared for this reaction: a 6 and 12% Ni dispersed into a nonstoichiometric magnesium aluminate (Ni-Mg-Al with spinel structure; b Ni-Raney catalyst. Both types of catalysts were active for (--menthone and (+-isomenthone hydrogenation. Lower conversion but higher selectivity to (--menthol was obtained with Ni-Mg-Al catalysts. However, they rapidly lost their activity. Instead Ni-Raney catalysts kept its original activity even after several hydrogenation runs.

  10. Characterization of Thioether-Linked Protein Adducts of DNA Using a Raney-Ni Mediated Desulfurization Method and Liquid Chromatography-Electrospray-Tandem Mass Spectrometry

    Science.gov (United States)

    Chowdhury, Goutam; Guengerich, F. Peter

    2015-01-01

    This unit contains a complete procedure for the detection and structural characterization of DNA protein crosslinks (DPCs). The procedure also describes an approach for the quantitation of the various structurally distinct DPCs. Although various methods have been described in the literature for labile DPCs, characterization of non-labile adducts remain a challenge. Here we present a novel approach for characterization of both labile and non-labile adducts by the use of a combination of chemical, enzymatic, and mass spectrometric approaches. A Raney Ni-catalyzed reductive desulfurization method was used for removal of the bulky peptide adducts, enzymatic digestion was used to digest the protein to smaller peptides and DNA to nucleosides, and finally LC-ESI-tandem mass spectrometry (MS) was utilized for detection and characterization of nucleoside adducts. PMID:25754888

  11. Energetic Mapping of Ni Catalysts by Detailed Kinetic Modeling

    DEFF Research Database (Denmark)

    Bjørgum, Erlend; Chen, De; Bakken, Mari G.

    2005-01-01

    Temperature-programmed desorption (TPD) of CO has been performed on supported and unsupported nickel catalysts. The unsupported Ni catalyst consists of a Ni(14 13 13) single crystal which has been studied under ultrahigh vacuum conditions. The desorption energy for CO at low CO surface coverage w...... nicely with literature values, providing useful information for identifying active sites on supported Ni catalysts....

  12. Liquid phase in situ hydrodeoxygenation of biomass-derived phenolic compounds to hydrocarbons over bifunctional catalysts

    Science.gov (United States)

    Junfeng Feng; Chung-yun Hse; Zhongzhi Yang; Kui Wang; Jianchun Jiang; Junming Xu

    2017-01-01

    The objective of this study was to find an effective method for converting renewable biomass-derived phenolic compounds into hydrocarbons bio-fuel via in situ catalytic hydrodeoxygenation. The in situ hydrodeoxygenation of biomass-derived phenolic compounds was carried out in methanol-water solvent over bifunctional catalysts of Raney Ni and HZSM-5 or H-Beta. In the in...

  13. Reduction of a Ni/Spinel Catalyst for Methane Reforming

    DEFF Research Database (Denmark)

    Kehres, Jan; Andreasen, Jens Wenzel; Fløystad, Jostein Bø

    2015-01-01

    A nickel/spinel (Ni/MgAl2O4) catalyst, w(Ni) = 22 wt%, was investigated in situ during reduction with wide angle X-ray scattering (WAXS) in a laboratory setup and with anomalous small angle X-ray scattering (ASAXS) at a synchrotron source. Complementary high resolution transmission electron...... microscopy (HRTEM) was performed on the fresh catalyst sample. The Ni particles in the fresh catalyst sample were observed to exhibit a Ni/NiO core/shell structure. A decrease of the Ni lattice parameter is observed during the reduction in a temperature interval from 413 – 453 K, which can be related...

  14. Influence of RANEY Nickel on the Formation of Intermediates in the Degradation of Lignin

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    Daniel Forchheim

    2012-01-01

    Full Text Available Lignin forms an important part of lignocellulosic biomass and is an abundantly available residue. It is a potential renewable source of phenol. Liquefaction of enzymatic hydrolysis lignin as well as catalytical hydrodeoxygenation of the main intermediates in the degradation of lignin, that is, catechol and guaiacol, was studied. The cleavage of the ether bonds, which are abundant in the molecular structure of lignin, can be realised in near-critical water (573 to 673 K, 20 to 30 MPa. Hydrothermal treatment in this context provides high selectivity in respect to hydroxybenzenes, especially catechol. RANEY Nickel was found to be an adequate catalyst for hydrodeoxygenation. Although it does not influence the cleavage of ether bonds, RANEY Nickel favours the production of phenol from both lignin and catechol. The main product from hydrodeoxygenation of guaiacol with RANEY Nickel was cyclohexanol. Reaction mechanism and kinetics of the degradation of guaiacol were explored.

  15. TEORES DE DIMETIL SULFETO ESTIMADOS PELO MÉTODO NÍQUEL-RANEY E ACEITABILIDADE DE AMOSTRAS DE CACHAÇA Dimethyl sulfide contents estimated by Ni-Raney method and “cachaça” samples acceptability.

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    J. F. A. TOLEDO

    2008-08-01

    Full Text Available

    O defeito sensorial das aguardentes de cana destiladas na ausência de cobre já foi relacionado com a presença do dimetil sulfeto (DMS, o que revela a importância de identificar os teores deste composto eventualmente presente nesta bebida. Considerando-se, porém, o custo relativamente elevado dos métodos de cromatografia de fase gasosa até agora utilizados na determinação do DMS, foi objetivo deste trabalho avaliar a possível utilização do método de Níquel-Raney como forma de controlar o referido defeito. Nesse sentido foi estudada a relação entre os teores de DMS estimados pelo método proposto, com sua influência sensorial avaliada através de testes de aceitação. Os resultados obtidos permitiram concluir que mesmo em concentrações abaixo de 5mg/L, os testes sensoriais revelam haver alta correlação entre os teores de DMS, determinados pelo método de Níquel-Raney com a diminuição da qualidade sensorial das amostras avaliadas. Os resultados obtidos permitem propor o método de Níquel-Raney como uma opção válida no controle da presença de DMS na cachaça e assim, prevenir efeitos negativos na qualidade sensorial do produto final.

    The sensory defect of “cachaça”, when distilled in absence of copper, had been already related to dimethyl sulphide levels, pointing out the importance to control its contents in this beverage. Considering the relatively higher costs of the gas-chromatography techniques, the aim of this work was to evaluate the possible use of the Níquel-Raney method, to control the dimethyl sulphide contents. In this way, the dimethyl sulphide contents (estimated by Níquel-Raney method and its sensory deffect evaluated by acceptability sensory tests, were compared. The results showed that

  16. Ni Catalysts Supported on Modified Alumina for Diesel Steam Reforming

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    Antonios Tribalis

    2016-01-01

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

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

    DEFF Research Database (Denmark)

    Wang, Ze; Zeng, Ying; Lin, Weigang

    2017-01-01

    performance improved. If gaseous hydrogen was used as the hydrogen source the activity of Ni/Al2O3 was pretty high. CO2 was found poisonous to the catalysis, due to the competitive adoption of phenol with CO2. If formic acid was replaced by methanol, the catalyst performance improved remarkably, with major...... products of cyclohexanone and cyclohexanol. The better effect of methanol enlightened the application of the supported Ni catalyst in in-situ hydrodeoxygenation of phenol....

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

    DEFF Research Database (Denmark)

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

    2007-01-01

    200-300 degrees C, and characterized using elemental analysis, N-2 physisorption measurements, XRD and TEM. Optimization of the catalyst performance was made by varying the Ni:Fe ratio, the total metal loading and the support material. For both support materials, the bimetallic catalysts...

  19. Metallic Ni3 P/Ni Co-Catalyst To Enhance Photocatalytic Hydrogen Evolution.

    Science.gov (United States)

    Zhao, Jun Jie; Liu, Peng Fei; Wang, Yu Lei; Li, Yu Hang; Zu, Meng Yang; Wang, Chong Wu; Wang, Xue Lu; Fang, Li Jun; Zeng, Hui Dan; Yang, Hua Gui

    2017-11-27

    Metallic Ni3 P/Ni can be used as a co-catalyst to replace noble metal Pt for efficient photocatalytic hydrogen evolution, due to its excellent trapping-electron ability. The applications of metallic Ni3 P/Ni co-catalyst on CdS, Zn0.5 Cd0.5 S, TiO2 (Degussa P25) and g-C3 N4 are further confirmed, indicating its versatile applicability nature like Pt. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  20. Synthesis, characterization and catalytic application of Ni catalysts ...

    Indian Academy of Sciences (India)

    TEM micrographs of nickel catalysts revealed particles in the size range of 10–30 nm. The Ni/Al 2 O 3 –ZrO 2 catalysts were tested in the steam reforming reaction of ethanol (SRE) at 500 ∘ C, and the obtained results suggest that the differences in catalytic activities depended on the content of ZrO 2 . The selectivity towards ...

  1. Raney Distributions and Random Matrix Theory

    Science.gov (United States)

    Forrester, Peter J.; Liu, Dang-Zheng

    2015-03-01

    Recent works have shown that the family of probability distributions with moments given by the Fuss-Catalan numbers permit a simple parameterized form for their density. We extend this result to the Raney distribution which by definition has its moments given by a generalization of the Fuss-Catalan numbers. Such computations begin with an algebraic equation satisfied by the Stieltjes transform, which we show can be derived from the linear differential equation satisfied by the characteristic polynomial of random matrix realizations of the Raney distribution. For the Fuss-Catalan distribution, an equilibrium problem characterizing the density is identified. The Stieltjes transform for the limiting spectral density of the singular values squared of the matrix product formed from inverse standard Gaussian matrices, and standard Gaussian matrices, is shown to satisfy a variant of the algebraic equation relating to the Raney distribution. Supported on , we show that it too permits a simple functional form upon the introduction of an appropriate choice of parameterization. As an application, the leading asymptotic form of the density as the endpoints of the support are approached is computed, and is shown to have some universal features.

  2. Hydrogenation of Tetralin over Supported Ni and Ir Catalysts

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    Dipali P. Upare

    2013-01-01

    Full Text Available Selective hydrogenation and ring opening (SRO of tetrahydronaphthalene (tetralin was studied over nickel and iridium supported catalysts in the context of the removal of polynuclear aromatics from diesel fuel. The tetralin hydrogenation was carried out in a fixed-bed reactor at 270°C, using H2 pressure of 30 bars, WHSV of 2.3 h−1, and H2/feed molar ratio of 40; the resultant products were analyzed by GC and GC-MS. The Ir/SiO2 catalyst gave 85% of tetralin conversion and 75.1% of decalin products selectivity whereas Ni/SiO2 catalyst showed an unprecedented high catalytic performance with 88.3% of tetralin conversion and 93% of decalin products selectivity. The catalysts were characterized by using different characterization techniques such as XRD, TPR, and HR-TEM to know the physicochemical properties as well as active sites in the catalysts.

  3. Production Hydrogen And Nanocarbon Via Methane Decomposition Using Ni-Based Catalysts. Effect Of Acidity And Catalyst Diameter

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    Widodo Purwanto

    2010-10-01

    Full Text Available Objectives of this research are mainly to study impacts of acidity strength (by varying amount of precipitant and loading Al-Si and the effect of nickel particle size (by varying calcinations temperature on decomposition reaction performances. In this research, high-nickel-loaded catalyst is prepared with two methods. Ni-Cu/Al catalysts were prepared with co-precipitation method. While the Ni-Cu/Al-Si catalyst were prepared by combined co-precipitation and sol-gel method. The direct cracking of methane was performed in 8mm quartz fixed bed reactor at atmospheric pressure and 500-700°C. The main  results showed that the Al content of catalyst increases with the increasing amount of precipitant. The activity of catalyst increases with the increasing of catalyst's acidity to the best possible point, and then increasing of acidity will reduce the activity of catalyst. Ni-Cu/4Al and Ni-Cu/11Al deactivated in a  very short time hence produced fewer amount of nanocarbon, while Ni-Cu/15Al was active in a very  long period. The most effective catalyst is Ni-Cu/22Al, which produced the biggest amount of nanocarbon (4.15 g C/g catalyst. Ni catalyst diameter has significant effect on reaction performances mainly  methane conversion and product yield. A small Ni crystal size gave a high methane conversion, a fast deactivation and a low carbon yield. Large Ni particle  diameter yielded a slow decomposition and low methane conversion. The highest methane  conversion was produced by catalyst diameter of 4 nm and maximum yield of carbon of 4.08 g C/ g catalyst was achieved by 15.5 nm diameter of Ni catalyst.

  4. Hydrogenation of Ethyl Acetate to Ethanol over Ni-Based Catalysts Obtained from Ni/Al Hydrotalcite-Like Compounds

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    Longfei Jiang

    2010-07-01

    Full Text Available A series of Ni-based catalysts were prepared using hydrogen reduction of Ni/Al hydrotalcite-like compounds (Ni/Al HTlcs synthesized by coprecipitation. The physico-chemical properties of Ni/Al hydrotalcite-like compounds and the corresponding Ni-based catalysts were characterized using inductively coupled plasma (ICP, BET surface areas, X-ray diffraction (XRD, Fourier transform infrared (FTIR spectroscopy and scanning electron microscopy (SEM techniques. The results indicated that Ni/Al HTlcs with layered structures could be successfully prepared by the coprecipitation method, and the characteristic HTlcs reflections were also observed in the XRD analysis. The NiO and Ni0 phases were identified in all Ni-based catalysts, which displayed randomly interconnected pores and no layer structures. In addition, the studies also found the Ni/Al HTlcs and Ni-based catalysts had high specific surface areas, low pore volumes and low pore diameters. The catalytic hydrogenation of ethyl acetate to ethanol with Ni-based catalysts was also investigated. Among the studied catalysts, RE1NASH-110-3 showed the highest selectivity and yield of ethyl acetate to ethanol, which were 68.2% and 61.7%, respectively. At the same time, a major by-product, butyl acetate, was formed due to an ester-exchange reaction. A proposed hydrogenation pathway for ethyl acetate over Ni-based catalysts was suggested.

  5. Glycerol Steam Reforming Over Ni-Fe-Ce/Al2O3 Catalyst: Effect of Cerium.

    Science.gov (United States)

    Go, Gwang-Sub; Go, Yoo-Jin; Lee, Hong-Joo; Moon, Dong-Ju; Park, Nam-Cook; Kim, Young-Chul

    2016-02-01

    In this work, hydrogen production from glycerol by steam reforming was studied using Ni-metal oxide catalysts. Ni-based catalyst becomes deactivated during steam reforming reactions because of coke deposits and sintering. Therefore, the aim of this study was to reduce carbon deposits and sintering on the catalyst surface by adding a promoter. Ni-metal oxide catalysts supported on Al2O3 were prepared via impregnation method, and the calcined catalyst was reduced under H2 flow for 2 h prior to the reaction. The characteristics of the catalysts were examined by XRD, TPR, TGA, and SEM. The Ni-Fe-Ce/Al2O3 catalyst, which contained less than 2 wt% Ce, showed the highest hydrogen selectivity and glycerol conversion. Further analysis of the catalysts revealed that the Ni-Fe-Ce/Al2O3 catalyst required a lower reduction temperature and produced minimum carbon deposit.

  6. Structural study of radiolytic catalysts Ni-Ce/Al2O3 and Ni-Pt/Al2O3

    Science.gov (United States)

    Seridi, F.; Chettibi, S.; Keghouche, N.; Beaunier, P.; Belloni, J.

    2017-01-01

    Ni-Ce and Ni-Pt bimetallic catalysts supported over α-Al2O3 are synthesized by using co-impregnation method, and then reduced, each via radiolytic process or thermal H2-treatment. For Ni-Ce/Al2O3, the structural study reveals that Ce is alloyed with Ni as Ce2Ni7 nanoparticles in the radiation-reduced catalysts, while it segregates to the surface in the form of CeO2 in the H2-reduced catalysts. For Ni-Pt/Al2O3 radiolytic catalysts, Ni, Pt, NiPt and Ni3Pt nanoparticles, which size is 3.5 nm, are observed. When the radiation-reduced samples are tested in the benzene hydrogenation, they both display high conversion rate. However, the Ni-Pt/Al2O3 is more efficient than Ni-Ce/Al2O3. The performance of the catalysts is correlated with the high dispersion of the metal and the presence of intermetallic Ni-Pt and Ni-Ce phases. It is compared to that of other radiolytic monometallic/oxide catalysts of the literature.

  7. PREPARATION AND CHARACTERIZATION THE NON-SULFIDED METAL CATALYST: Ni/USY and NiMo/USY

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    Khoirina Dwi Nugrahaningtyas

    2010-06-01

    Full Text Available The two-new catalysts had been prepared by using the impregnation method according to Nugrahaningtyas [6] and Li [4]. One catalyst is of Nickel (Ni, supported on Ultra Stable Zeolite Y (USY, whereas the other one is NiMo supported on same supporting agent. These new catalysts are expected to be more effective when applied on the hydrotreatment reaction in standpoint of its capabilities on removing the unwanted-heteroatom. Characterization those two types of catalysts then carried out by using the criteria of acidity, porosity and, metal content. The result shows that these non-sulfide catalysts have several good characters that supporting their usefulness in hydrotreatment-catalytic reaction. In addition, catalyst NiMo/USY - 1 performs many ideal criteria as the best functional catalyst.   Keywords: Non-sulfided Catalyst, hydro-treating, preparation, characterization

  8. Production Hydrogen and Nanocarbon Via Methane Decomposition Using Ni-based Catalysts. Effect of Acidity and Catalyst Diameter

    OpenAIRE

    Widodo W. Purwanto; M Nasikin; E Saputra; Song, L.

    2005-01-01

    Objectives of this research are mainly to study impacts of acidity strength (by varying amount of precipitant and loadingAl-Si) and the effect of nickel particle size (by varying calcinations temperature) on decomposition reactionperformances. In this research, high-nickel-loaded catalyst is prepared with two methods. Ni-Cu/Al catalysts wereprepared with co-precipitation method. While the Ni-Cu/Al-Si catalyst were prepared by combined co-precipitation andsol-gel method. The direct cracking of...

  9. Hydrogenation of xylose to xylitol on sponge nickel catalyst: a study of the process and catalyst deactivation kinetics

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    Mikkola J.-P.

    2003-01-01

    Full Text Available The kinetics of hydrogenation of xylose to xylitol on a sponge nickel catalyst (commonly referred to as Raney Ni catalyst and of catalyst deactivation were studied. Plausible explanations for the decrease in catalytic activity by means of surface studies, nitrogen adsorption and thermogravimetric analyses of the fresh and spent catalysts are presented. The kinetic parameters of the process were estimated by the use of a semi-competitive model, which allows full competition between the organic species and the hydrogen atoms for the adsorption sites on the catalyst surface (competitive case. In the model, a competitiveness factor (alpha is introduced to take into account that even after complete coverage of the surface by the organic species, interstitial sites remain for the adsorption of the hydrogen atoms.

  10. Enhanced Activity of Supported Ni Catalysts Promoted by Pt for Rapid Reduction of Aromatic Nitro Compounds

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    Huishan Shang

    2016-06-01

    Full Text Available To improve the activities of non-noble metal catalysts is highly desirable and valuable to the reduced use of noble metal resources. In this work, the supported nickel (Ni and nickel-platinum (NiPt nanocatalysts were derived from a layered double hydroxide/carbon composite precursor. The catalysts were characterized and the role of Pt was analysed using X-ray diffraction (XRD, high-resolution transmission electron microscopy (HRTEM, energy dispersive X-ray spectroscopy (EDS mapping, and X-ray photoelectron spectroscopy (XPS techniques. The Ni2+ was reduced to metallic Ni0 via a self-reduction way utilizing the carbon as a reducing agent. The average sizes of the Ni particles in the NiPt catalysts were smaller than that in the supported Ni catalyst. The electronic structure of Ni was affected by the incorporation of Pt. The optimal NiPt catalysts exhibited remarkably improved activity toward the reduction of nitrophenol, which has an apparent rate constant (Ka of 18.82 × 10−3 s−1, 6.2 times larger than that of Ni catalyst and also larger than most of the reported values of noble-metal and bimetallic catalysts. The enhanced activity could be ascribed to the modification to the electronic structure of Ni by Pt and the effect of exposed crystal planes.

  11. Metal oxides modified NiO catalysts for oxidative dehydrogenation of ethane to ethylene

    KAUST Repository

    Zhu, Haibo

    2014-06-01

    The sol-gel method was applied to the synthesis of Zr, Ti, Mo, W, and V modified NiO based catalysts for the ethane oxidative dehydrogenation reaction. The synthesized catalysts were characterized by XRD, N2 adsorption, SEM and TPR techniques. The results showed that the doping metals could be highly dispersed into NiO domains without the formation of large amount of other bulk metal oxide. The modified NiO materials have small particle size, larger surface area, and higher reduction temperature in contrast to pure NiO. The introduction of group IV, V and VI transition metals into NiO decreases the catalytic activity in ethane ODH. However, the ethylene selectivity is enhanced with the highest level for the Ni-W-O and Ni-Ti-O catalysts. As a result, these two catalysts show improved efficiency of ethylene production in the ethane ODH reaction. © 2014 Elsevier B.V. All rights reserved.

  12. Highly coke-resistant ni nanoparticle catalysts with minimal sintering in dry reforming of methane.

    Science.gov (United States)

    Han, Joung Woo; Kim, Chanyeon; Park, Jun Seong; Lee, Hyunjoo

    2014-02-01

    Nickel catalysts are typically used for hydrogen production by reforming reactions. Reforming methane with carbon dioxide, called dry reforming of methane (DRM), is a good way to produce hydrogen or syngas (a mixture of hydrogen and carbon monoxide) from two notable greenhouse gases. However, Ni catalysts used for DRM suffer from severe coke deposition. It has been known that small Ni nanoparticles are advantageous to reduce coke formation, but the high reaction temperature of DRM (800 °C) inevitably induces aggregation of the nanoparticles, leading to severe coke formation and degraded activity. Here, we develop highly coke-resistant Ni catalysts by immobilizing premade Ni nanoparticles of 5.2 nm in size onto functionalized silica supports, and then coating the Ni/SiO2 catalyst with silica overlayers. The silica overlayers enable the transfer of reactants and products while preventing aggregation of the Ni nanoparticles. The silica-coated Ni catalysts operate stably for 170 h without any degradation in activity. No carbon deposition was observed by temperature programmed oxidation (TPO), transmission electron microscopy (TEM), X-ray diffraction (XRD), and Raman spectroscopy. The Ni catalysts without silica coating show severe sintering after DRM reaction, and the formation of filamentous carbon was observed. The coke-resistant Ni catalyst is potentially useful in various hydrocarbon transformations. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

    Directory of Open Access Journals (Sweden)

    Laura Pastor-Pérez

    2015-03-01

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

  14. Hydrogen generation from decomposition of hydrous hydrazine over Ni-Ir/CeO2 catalyst

    OpenAIRE

    Dai, Hongbin; Zhong, Yujie; Wang, Ping

    2017-01-01

    The synthesis of highly active and selective catalysts is the central issue in the development of hydrous hydrazine (N2H4·H2O) as a viable hydrogen carrier. Herein, we report the synthesis of bimetallic Ni-Ir nanocatalyts supported on CeO2 using a one-pot coprecipitation method. A combination of XRD, HRTEM and XPS analyses indicate that the Ni-Ir/CeO2 catalyst is composed of tiny Ni-Ir alloy nanoparticles with an average size of around 4 nm and crystalline CeO2 matrix. The Ni-Ir/CeO2 catalyst...

  15. Various conformations of carbon nanocoils prepared by supported Ni-Fe/molecular sieve catalyst.

    Science.gov (United States)

    Yang, Shaoming; Chen, Xiuqin; Takeuchi, K; Motojima, Seiji

    2006-01-01

    The carbon nanocoils with various kinds of conformations were prepared by the catalytic pyrolysis of acetylene using the Ni metal catalyst supported on molecular Sieves which was prepared using Fe-containing kaolin as the raw material. There are four kinds of carbon nanocoils conformations produced by this catalyst. The influences of reaction temperature and gas conditions on the conformations of the nanocoils were investigated and the reasons of forming nano-size coils were discussed by comparison with pure Ni metal catalyst.

  16. Deactivation and Regeneration of Ni/ZA Catalyst in Hydrocracking of Polypropylene

    Directory of Open Access Journals (Sweden)

    Imam Khabib

    2014-07-01

    Full Text Available The phenomena of catalyst deactivation and the effects of regeneration method on the characteristics and activity of Ni/ZA catalyst after being used in a continuous cracking reaction of polypropylene have been studied. Ni/ZA catalyst was prepared using sonochemical method with total metal intake of 4%. Characteristics and activity of fresh, spent, and regenerated catalyst were evaluated to get a better understanding about the catalyst deactivation. Characteristics which have been observed include catalyst acidity, porosity, crystallinity, and surface morphology. Catalytic activity test of Ni/ZA catalyst on polypropylene cracking reaction at temperature of 500 °C with H2 flow rate of 20 mL/min and catalyst:feed ratio of 1:2 (w/w showed the decrease of some catalyst characteristics such as specific surface area, total pore volume, and acidity due to coke fouling over a five-times continuous experiment. Regeneration of catalyst with oxidation-reduction method has been able to increase the activity and acidity of catalyst up to 7.47% and 38.54%, respectively, compared to those of spent catalyst, while the catalyst surface area and total pore volume decreased up to 32.83% and 26.92%, respectively.

  17. Ni-Based Catalysts for the Hydrotreatment of Fast Pyrolysis Oil

    NARCIS (Netherlands)

    Ardiyanti, A. R.; Bykova, M. V.; Khromova, S. A.; Yin, W.; Venderbosch, R. H.; Yakovlev, V. A.; Heeres, Hero

    Catalytic hydrotreatment is an attractive technology to convert fast pyrolysis oil to stabilized oil products for co processing in conventional crude oil refinery units. We report here the use of novel bimetallic NiCu- and NiPd-based (Picula) catalysts characterized by a high Ni content (29-58 wt %)

  18. Alloyed Ni-Fe nanoparticles as catalysts for NH3 decomposition

    DEFF Research Database (Denmark)

    Simonsen, Søren Bredmose; Chakraborty, Debasish; Chorkendorff, Ib

    2012-01-01

    A rational design approach was used to develop an alloyed Ni-Fe/Al2O3 catalyst for decomposition of ammonia. The dependence of the catalytic activity is tested as a function of the Ni-to-Fe ratio, the type of Ni-Fe alloy phase, the metal loading and the type of oxide support. In the tests with high...

  19. Development of Non-Noble Metal Ni-Based Catalysts for Dehydrogenation of Methylcyclohexane

    KAUST Repository

    Al-ShaikhAli, Anaam H.

    2016-11-30

    Liquid organic chemical hydride is a promising candidate for hydrogen storage and transport. Methylcyclohexane (MCH) to toluene (TOL) cycle has been considered as one of the feasible hydrogen carrier systems, but selective dehydrogenation of MCH to TOL has only been achieved using the noble Pt-based catalysts. The aim of this study is to develop non-noble, cost-effective metal catalysts that can show excellent catalytic performance, mainly maintaining high TOL selectivity achievable by Pt based catalysts. Mono-metallic Ni based catalyst is a well-known dehydrogenation catalyst, but the major drawback with Ni is its hydrogenolysis activity to cleave C-C bonds, which leads to inferior selectivity towards dehydrogenation of MCH to TOL. This study elucidate addition of the second metal to Ni based catalyst to improve the TOL selectivity. Herein, ubiquitous bi-metallic nanoparticles catalysts were investigated including (Ni–M, M: Ag, Zn, Sn or In) based catalysts. Among the catalysts investigated, the high TOL selectivity (> 99%) at low conversions was achieved effectively using the supported NiZn catalyst under flow of excess H2. In this work, a combined study of experimental and computational approaches was conducted to determine the main role of Zn over Ni based catalyst in promoting the TOL selectivity. A kinetic study using mono- and bimetallic Ni based catalysts was conducted to elucidate reaction mechanism and site requirement for MCH dehydrogenation reaction. The impact of different reaction conditions (feed compositions, temperature, space velocity and stability) and catalyst properties were evaluated. This study elucidates a distinctive mechanism of MCH dehydrogenation to TOL reaction over the Ni-based catalysts. Distinctive from Pt catalyst, a nearly positive half order with respect to H2 pressure was obtained for mono- and bi-metallic Ni based catalysts. This kinetic data was consistent with rate determining step as (somewhat paradoxically) hydrogenation

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

    KAUST Repository

    Alotaibi, Raja

    2015-07-08

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

  1. Catalysts characteristics of Ni/YSZ core-shell according to plating conditions using electroless plating

    Science.gov (United States)

    Park, Hyun-Wook; Jang, Jae-Won; Lee, Young-Jin; Kim, Jin-Ho; Jeon, Dae-Woo; Lee, Jong-Heun; Hwang, Hae-jin; Lee, Mi-Jai

    2017-11-01

    This study aims to develop an anode catalyst for a solid oxide fuel cell (SOFC) using electroless nickel plating. We have proposed a new method for electroless plating of Ni metal on yttria-stabilized zirconia (YSZ) particles. We examine the uniformity of the Ni layer on the plated core-shell powder, in addition to the content of Ni and the reproducibility of the plating. We have also evaluated the carbon deposition rate and characteristics of the SOFC anode catalyst. To synthesize Ni-plated YSZ particles, the plated powder is heat-treated at 1200 °C. The resultant particles, which have an average size of 50 μm, were subsequently used in the experiment. The size of the Ni particles and the Ni content both increase with increasing plating temperature and plating time. The X-ray diffraction pattern reveals the growth of Ni particles. After heat-treatment, Ni is oxidized to NiO, leading to the co-existence of Ni and NiO; Ni3P is also observed due to the presence of phosphorous in the plating solution. Following heat treatment for 1 h at 1200 °C, Ni is mostly oxidized to NiO. The carbon deposition rate of the reference YSZ powder is 135%, while that of the Ni-plated YSZ is 1%-6%.

  2. Steam Reforming of Glycerol Over Nano Size Ni-Ce/LaAlO3 Catalysts.

    Science.gov (United States)

    Kim, Seong-Hak; Go, Yoo-Jin; Park, Nam-Cook; Kim, Jong-Ho; Kim, Young-Chul; Moon, Dong-Ju

    2015-01-01

    In this work, hydrogen production from glycerol by Steam Reforming (SR) was studied by Ni-Ce catalysts supported on LaAlO3 perovskite in order to effect of the cerium loading amount and the reaction conditions. Nano size Ni-Ce/LaAlO3 catalysts were prepared by precipitation method. The structure of the catalysts was characterized by XRD analysis. The morphology, dispersion and the reduction properties of catalysts was examined by SEM, TEM, H2-chemisorption and TPR, respectively. It was found that 15 wt% Ni-5 wt% Ce/LaAlO3 catalyst showed the highest glycerol conversion and hydrogen selectivity. In addition, the catalyst also showed the high carbon dioxide selectivity and the lowest methane selectivity. The results indicate that the catalyst promotes methane reforming reaction. The highest activity in the 15 wt% Ni-5 wt% Ce/LaAlO3 was attributed to the proper cerium loading amount. Moreover, the lowest metal crystal size and rise in active site were found to have an effect on catalytic activity and hydrogen selectivity. The 15 wt% Ni-5 wt% Ce/LaAlO3 catalyst exhibited excellent performance with respect to hydrogen production at reaction temperature of 450 degrees C, at atmospheric pressure, 20 wt% glycerol solution and GHSV = 6,000 mL/g-cat x hr.

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

    DEFF Research Database (Denmark)

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

    2007-01-01

    addition was a rapid deactivation of the catalyst due to an enhanced gum carbon formation on the Ni crystals. Contrary to this, the effect of K addition was a prolonged resistance against carbon formation and therefore against deactivation. The Ru catalyst operates better than all the Ni catalysts...... for the production of hydrogen is investigated, along with quantitative and qualitative determinations of carbon formation on the catalysts by TPO and TEM experiments. A Ru/ MgAl2O4 catalyst, a Ni/MgAl2O4 catalyst as well as Ag-and K-promoted Ni/ MgAl2O4 catalysts were studied. The operating temperature was between...... 673 and 873 K, and a 25 vol% ethanol -water mixture was employed. Deactivation of the catalysts by carbon formation is the main obstacle for industrial use of this process. Carbon formation was found to be highly affected by the operating temperature and the choice of catalyst. The effect of Ag...

  4. Preparation and characterization of Ni-based perovskite catalyst for steam CO2 reforming of methane.

    Science.gov (United States)

    Yang, Eun-Hyeok; Kim, Sang Woo; Ahn, Byong Song; Moon, Dong Ju

    2013-06-01

    Steam CO2 reforming of methane was investigated over Ni-based perovskite catalyst to produce desired H2/CO ratio by adjusting the feed ratio of CH4, CO2 and H2O for floating GTL process application. La modified perovskites were prepared by the Pechini method and calcined in air and the Ni-based catalysts were prepared by dispersing Ni on the La modified perovskite by an incipient wetness impregnation. The catalysts before and after the reaction were characterized by N2 physisoprtion, CO chemisoprtion, XRD, TPR and SEM techniques. To control desired H2/CO ratio, simulation for SCR was carried out by Aspen plus, and product distribution for SCR was investigated in a fixed bed reactor system using feed ratio estimated by simulation. The Ni-based perovskite catalysts were found to give CH4 and CO2 conversions of up to 82% and 60% respectively to yield a H2/CO product ratio close to 2.

  5. Methane decomposition over high-loaded Ni-Cu-SiO{sub 2} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Li, Jiamao; Zhao, Linjie; He, Jianchao; Dong, Liang; Xiong, Liangping; Du, Yang; Yang, Yong; Wang, Heyi, E-mail: hywang@caep.cn; Peng, Shuming, E-mail: pengshuming@caep.cn

    2016-12-15

    Graphical abstract: Methane decomposition-regeneration with air cycles over 65%Ni-20%Cu-10%SiO{sub 2} catalysts. - Highlights: • Methane decomposition over Ni-Cu-SiO{sub 2} was studied. • The deactivated catalysts were regenerated by air. • Introduction of Cu could enhance the catalytic performance of Ni-SiO{sub 2}. • The increase of the Ni-Cu particle influences the performance of the catalysts. - Abstract: The performance of Ni-SiO{sub 2} and Ni-Cu-SiO{sub 2} during repeated catalytic decomposition of methane (CDM) reactions and subsequent regeneration of the deactivated catalysts with air has been studied. The catalytic activity of the 75%Ni-25%SiO{sub 2} catalyst in the second and third CDM was lower than that during the first, while the lifetime of the catalyst did not change significantly. Both the lifetime and the catalytic activity of 65%Ni-10%Cu-25%SiO{sub 2} in the second and third CDM reactions decreased significantly. 55%Ni-20%Cu-25%SiO{sub 2} showed better performance than the other two catalysts, and its activity and lifetime did not change significantly until the third CDM reaction. The hydrogen yields of 55%Ni-20%Cu-25%SiO{sub 2} were 56.8 gH{sub 2}/gcat., 42.8 gH{sub 2}/gcat., and 2.4 gH{sub 2}/gcat. for the first, second, and third CDM reactions, respectively. Spherical carbon structures were observed on the catalysts following all three CDM reactions over 75%Ni-25%SiO{sub 2}. However, similar carbon structures were only observed following the second and third CDM over 65%Ni-10%Cu-25%SiO{sub 2}, and only following the third cycle with 55%Ni-20%Cu-25%SiO{sub 2}. The formation of spherical carbon during the repeated CDM reactions strongly influenced the performance of the catalysts.

  6. Mechanistic aspects of the ethanol steam reforming reaction for hydrogen production on Pt, Ni, and PtNi catalysts supported on gamma-Al2O3.

    Science.gov (United States)

    Sanchez-Sanchez, Maria Cruz; Navarro Yerga, Rufino M; Kondarides, Dimitris I; Verykios, Xenophon E; Fierro, Jose Luis G

    2010-03-25

    Mechanistic aspects of ethanol steam reforming on Pt, Ni, and PtNi catalysts supported on gamma-Al(2)O(3) are investigated from the analysis of adsorbed species and gas phase products formed on catalysts during temperature-programmed desorption of ethanol and during ethanol steam reforming reaction. DRIFTS-MS analyses of ethanol decomposition and ethanol steam reforming reactions show that PtNi and Ni catalysts are more stable than the Pt monometallic counterpart. Ethanol TPD results on Ni, Pt, and NiPt catalysts point to ethanol dehydrogenation and acetaldehyde decomposition as the first reaction pathways of ethanol steam reforming over the studied catalysts. The active sites responsible for the acetaldehyde decomposition are easily deactivated in the first minutes on-stream by carbon deposits. For Ni and PtNi catalysts, a second reaction pathway, consisting in the decomposition of acetate intermediates formed over the surface of alumina support, becomes the main reaction pathway operating in steam reforming of ethanol once the acetaldehyde decomposition pathway is deactivated. Taking into account the differences observed in the mechanism of ethanol decomposition, the better stability observed for PtNi catalyst is proposed to be related with a cooperative effect between Pt and Ni activities together with the enhanced ability of Ni to gasify the methyl groups formed by decomposition of acetate species. On the contrary, monometallic catalysts are believed to dehydrogenate these methyl groups forming coke that leads to deactivation of metal particles.

  7. Enhanced sulfur resistance of Ni/SiO2 catalyst for methanation via the plasma decomposition of nickel precursor.

    Science.gov (United States)

    Yan, Xiaoliang; Liu, Yuan; Zhao, Binran; Wang, Yong; Liu, Chang-jun

    2013-08-07

    A Ni/SiO2 catalyst was prepared by the plasma decomposition of a nickel precursor via dielectric barrier discharge (DBD). The obtained Ni/SiO2 catalyst shows an enhanced H2S resistance for methanation of syngas (CO + H2). The plasma decomposition has a significant influence on the structural property of Ni/SiO2. The plasma decomposed catalyst shows less defect sites on Ni particles. The formation of Ni-sulfur species was effectively inhibited. The mechanism of H2S poisoning on different catalysts with and without plasma decomposition was also discussed according to the reaction temperature.

  8. 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.

  9. Coking of Ni-based catalysts at the process of methane conversion with carbon dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Rudnitsky, L.A.; Soboleva, T.N.; Korotkova, G.; Alexseev, A.M. [Institute for Nitrogen Industry, Moscow (Russian Federation)

    1995-12-31

    The process of methane conversion with carbon dioxide over Ni-based supported catalyst (NiSC) is followed by the reversible reaction of carbon formation on the NiSC at certain conditions. This reaction is of interest as a model for investigation of coking reaction (CR) and it`s reverse one - gasification (GR) on different types of NiSC. The study of dynamics of CR and GR was carried out with thermomicrobalance at the atmospheric pressure in methane - carbon dioxide mixture flow over previously reduced NiSC at linear temperature programming in heating and cooling regimes.

  10. NiO-PTA supported on ZIF-8 as a highly effective catalyst for hydrocracking of Jatropha oil

    Science.gov (United States)

    Liu, Jing; He, Jing; Wang, Luying; Li, Rong; Chen, Pan; Rao, Xin; Deng, Lihong; Rong, Long; Lei, Jiandu

    2016-01-01

    Nickel oxide (NiO) and phosphotungstic acid (PTA) supported on a ZIF-8 (NiO-PTA/ZIF-8) catalyst was first synthesized and it showed high activity and good selectivity for the hydrocracking of Jatropha oil. The catalyst was characterized by SEM, SEM-EDS, TEM, N2 adsorption, FT-IR, XRD and XPS. Compared with the NiO-PTA/Al2O3 catalyst, the selectivity of C15-C18 hydrocarbon increased over 36%, and catalytic efficiency increased 10 times over the NiO-PTA/ZIF-8 catalyst. The prepared NiO-PTA/ZIF-8 catalyst was stable for a reaction time of 104 h and the kinetic behavior was also analyzed. This catalyst was found to bypass the presulfurization process, showing promise as an alternative to sulfided catalysts for green diesel production. PMID:27020579

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

    DEFF Research Database (Denmark)

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

    2014-01-01

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

  12. Supercritical water gasification of microalga Nannochloropsis over supported Ni and Ru catalysts

    Science.gov (United States)

    Wijenayake, A. G. B. S. P.; Hassan, M.; Komiyama, M.

    2016-11-01

    Supercritical water gasification (SCWG) of a marine microalga Nannochloropsis was performed in the presence and the absence of supported Ru and Ni catalysts at 385 °C and 26 MPa using a batch reactor. The product gas of the non-catalytic reaction mainly comprised of CO2 while that of catalytic reaction produced CH4, CO2, H2 and some C2-C4 compounds. The addition of catalysts enhanced the decomposition and conversion (water-gas shift and methanation) reactions, consequently increasing the total gasification efficiency up to 92% for 60 min reaction time. Between the supported Ru and Ni catalysts, Ru resulted in higher gasification efficiency than Ni. Catalyst deactivation during SCWG of Nannochloropsis was also examined.

  13. Hydrogen generation from decomposition of hydrous hydrazine over Ni-Ir/CeO2 catalyst

    Directory of Open Access Journals (Sweden)

    Hongbin Dai

    2017-02-01

    Full Text Available The synthesis of highly active and selective catalysts is the central issue in the development of hydrous hydrazine (N2H4·H2O as a viable hydrogen carrier. Herein, we report the synthesis of bimetallic Ni-Ir nanocatalyts supported on CeO2 using a one-pot coprecipitation method. A combination of XRD, HRTEM and XPS analyses indicate that the Ni-Ir/CeO2 catalyst is composed of tiny Ni-Ir alloy nanoparticles with an average size of around 4 nm and crystalline CeO2 matrix. The Ni-Ir/CeO2 catalyst exhibits high catalytic activity and excellent selectivity towards hydrogen generation from N2H4·H2O at mild temperatures. Furthermore, in contrast to previously reported Ni-Pt catalysts, the Ni-Ir/CeO2 catalyst shows an alleviated requirement on alkali promoter to achieve its optimal catalytic performance.

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

    Directory of Open Access Journals (Sweden)

    Rodiansono Rodiansono

    2010-06-01

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

  15. Effect of Phosphine Doping and the Surface Metal State of Ni on the Catalytic Performance of Ni/Al2O3 Catalyst

    Directory of Open Access Journals (Sweden)

    Xiaoru Li

    2015-04-01

    Full Text Available Ni-based catalysts as replacement for noble metal catalysts are of particular interest in the catalytic conversion of biomass due to their cheap and satisfactory catalytic activity. The Ni/SiO2 catalyst has been studied for the hydrogenolysis of glycerol, and doping with phosphorus (P found to improve the catalytic performance significantly because of the formation of Ni2P alloys. However, in the present work we disclose a different catalytic phenomenon for the P-doped Ni/Al2O3 catalyst. We found that doping with P has a significant effect on the state of the active Ni species, and thus improves the selectivity to 1,2-propanediol (1,2-PDO significantly in the hydrogenolysis of glycerol, although Ni-P alloys were not observed in our catalytic system. The structure and selectivity correlations were determined from the experimental data, combining the results of X-ray diffraction (XRD, X-ray photoelectron spectroscopy (XPS, hydrogen temperature-programmed reduction (H2-TPR and ammonia temperature-programmed desorption (NH3-TPD. The presence of NiO species, formed from P-doped Ni/Al2O3 catalyst, was shown to benefit the formation of 1,2-PDO. This was supported by the results of the Ni/Al2O3 catalyst containing NiO species with incomplete reduction. Furthermore, the role the NiO species played in the reaction and the potential reaction mechanism over the P-doped Ni/Al2O3 catalyst is discussed. The new findings in the present work open a new vision for Ni catalysis and will benefit researchers in designing Ni-based catalysts.

  16. Hydrogen production by ethanol steam reforming over Cu-Ni supported catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Vizcaino, A.J.; Carrero, A.; Calles, J.A. [Department of Chemical and Environmental Technology, Rey Juan Carlos University, Escuela Superior de Ciencias Experimentales y Tecnologia (ESCET), c/ Tulipan s/n, 28933 Mostoles (Spain)

    2007-07-15

    In the present work, Cu-Ni supported catalysts were tested in ethanol steam reforming reaction. Two commercial amorphous solids (SiO{sub 2} and {gamma}-Al{sub 2}O{sub 3}) and three synthesized materials (MCM-41, SBA-15 and ZSM-5 nanocrystalline) were used as support. A series of Cu-Ni/SiO{sub 2} catalysts with different Cu and Ni content were also prepared. It was found that aluminium containing supports favour ethanol dehydration to ethylene in the acid sites, which in turn, promotes the coke deactivation process. The highest hydrogen selectivity is achieved with the Cu-Ni/SBA-15 catalyst, due to a smaller metallic crystallite size. Nevertheless, the Cu-Ni/SiO{sub 2} catalyst showed the best catalytic performance, since a better equilibrium between high hydrogen selectivity and CO{sub 2}/CO{sub x} ratio is obtained. It was seen that nickel is the phase responsible for hydrogen production in a greater grade, although both CO production and coke deposition are decreased when copper is added to the catalyst. (author)

  17. An Alumina-Supported Ni-La-Based Catalyst for Producing Synthetic Natural Gas

    Directory of Open Access Journals (Sweden)

    Daniel E. Rivero-Mendoza

    2016-10-01

    Full Text Available LaNi5, known for its hydrogen storage capability, was adapted to the form of a metal oxide-supported (γ-Al2O3 catalyst and its performance for the Sabatier reaction assessed. The 20 wt % La-Ni/γ-Al2O3 particles were prepared via solution combustion synthesis (SCS and exhibited good catalytic activity, achieving a CO2 conversion of 75% with a high CH4 selectivity (98% at 1 atm and 300 °C. Characteristics of the La-Ni/γ-Al2O3 catalyst were identified at various stages of the catalytic process (as-prepared, activated, and post-reaction and in-situ DRIFTS was used to probe the reaction mechanism. The as-prepared catalyst contained amorphous surface La–Ni spinels with particle sizes <6 nm. The reduction process altered the catalyst make-up where, despite the reducing conditions, Ni2+-based particles with diameters between 4 and 20 nm decorated with LaOx moieties were produced. However, the post-reaction catalyst had particle sizes of 4–9 nm and comprised metallic Ni, with the LaOx decoration reverting to a form akin to the as-prepared catalyst. DRIFTS analysis indicated that formates and adsorbed CO species were present on the catalyst surface during the reaction, implying the reaction proceeded via a H2-assisted and sequential CO2 dissociation to C and O. These were then rapidly hydrogenated into CH4 and H2O.

  18. Structured Ni catalysts on porous anodic alumina membranes for methane dry reforming: NiAl 2 O 4 formation and characterization

    KAUST Repository

    Zhou, Lu

    2015-06-29

    This communication presents the successful design of a structured catalyst based on porous anodic alumina membranes for methane dry reforming. The catalyst with a strong Ni-NiAl2O4 interaction shows both excellent activity and stability. This journal is © The Royal Society of Chemistry.

  19. Interaction between Ni and HZSM-5 in aromatization-enhanced reactive adsorption desulfurization catalysts for FCC gasoline upgrading.

    Science.gov (United States)

    Zhao, Jinchong; Zhang, Lulu; She, Nannan; Liu, Yunqi; Chai, Yongming; Liu, Chenguang

    A compound catalyst (RA) consisted of Ni, ZnO and HZSM-5 with functions of reactive adsorption desulfurization (RADS) and olefin aromatization for fluid catalytic cracking (FCC) gasoline upgrading was prepared. X-ray powder diffraction (XRD), temperature-programmed reduction and low-temperature N2 adsorption were used to characterize the properties of the catalysts. Performance evaluation by FCC gasoline was carried out, and the result showed that the catalyst RA performed well in desulfurization and aromatization. For comparison, RADS catalyst (represented by DS) consisted of Ni and ZnO and aromatization catalyst (represented by Ar) consisted of HZSM-5 were prepared, respectively. They were combined in different ways to help investigating interaction between Ni and HZSM-5. Performance evaluated by FCC gasoline showed that catalyst RA performed best in desulfurization with a slight octane number loss. Interaction between Ni and HZSM-5 is a significant factor which influences the performance of the catalyst.

  20. Microwave-assisted Ni-La/γ-Al2O3 catalyst for benzene hydrogenation

    Science.gov (United States)

    Liu, Xianjun; Liu, Shuzhi; Xu, Peiqiang

    2017-11-01

    A series of Ni-La/γ-Al2O3 catalysts were prepared by adopting the methods of isometric impregnation and microwave impregnation. The catalysts were characterized with XRD, BET, and SEM, respectively. Inspecting the effects of adding La and the methods of impregnation on the hydrogenation activity of catalysts. The results show that adding a moderate amount of La promotes the dispersing of Ni on the carrier, the methods of microwave impregnation weaks the interaction between Ni and the carrier further, inhibits the formation of NiAl2O4, and the activity of catalyst prepared by the methods of microwave impregnation was significantly higher than that prepared by the methods of isometric impregnation. The hydrogenation activity of the Ni-La/γ-Al2O3 (WB) dipped with n(Ni): n(La) = 4: 1, microwave irradiation time 30 min with power 600W as well as calcined at 400°C exhibited the best performance. The conversion rate is 91.21% with reaction conditions: T = 160°C, p = 0.8 MPa, air speed 5 h-1, n(H2): n(benzene) = 2: 1.

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

    Science.gov (United States)

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

    2014-12-01

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

  2. Cooperativity and Dynamics Increase the Performance of NiFe Dry Reforming Catalysts.

    Science.gov (United States)

    Kim, Sung Min; Abdala, Paula Macarena; Margossian, Tigran; Hosseini, Davood; Foppa, Lucas; Armutlulu, Andac; van Beek, Wouter; Comas-Vives, Aleix; Copéret, Christophe; Müller, Christoph

    2017-02-08

    The dry reforming of methane (DRM), i.e., the reaction of methane and CO2 to form a synthesis gas, converts two major greenhouse gases into a useful chemical feedstock. In this work, we probe the effect and role of Fe in bimetallic NiFe dry reforming catalysts. To this end, monometallic Ni, Fe, and bimetallic Ni-Fe catalysts supported on a MgxAlyOz matrix derived via a hydrotalcite-like precursor were synthesized. Importantly, the textural features of the catalysts, i.e., the specific surface area (172-178 m(2)/gcat), pore volume (0.51-0.66 cm(3)/gcat), and particle size (5.4-5.8 nm) were kept constant. Bimetallic, Ni4Fe1 with Ni/(Ni + Fe) = 0.8, showed the highest activity and stability, whereas rapid deactivation and a low catalytic activity were observed for monometallic Ni and Fe catalysts, respectively. XRD, Raman, TPO, and TEM analysis confirmed that the deactivation of monometallic Ni catalysts was in large due to the formation of graphitic carbon. The promoting effect of Fe in bimetallic Ni-Fe was elucidated by combining operando XRD and XAS analyses and energy-dispersive X-ray spectroscopy complemented with density functional theory calculations. Under dry reforming conditions, Fe is oxidized partially to FeO leading to a partial dealloying and formation of a Ni-richer NiFe alloy. Fe migrates leading to the formation of FeO preferentially at the surface. Experiments in an inert helium atmosphere confirm that FeO reacts via a redox mechanism with carbon deposits forming CO, whereby the reduced Fe restores the original Ni-Fe alloy. Owing to the high activity of the material and the absence of any XRD signature of FeO, it is very likely that FeO is formed as small domains of a few atom layer thickness covering a fraction of the surface of the Ni-rich particles, ensuring a close proximity of the carbon removal (FeO) and methane activation (Ni) sites.

  3. Relationship between surface property and catalytic application of amorphous NiP/Hβ catalyst for n-hexane isomerization

    Science.gov (United States)

    Chen, Jinshe; Duan, Zunbin; Song, Zhaoyang; Zhu, Lijun; Zhou, Yulu; Xiang, Yuzhi; Xia, Daohong

    2017-12-01

    The amorphous NiP nanoparticles were synthesized and a novel amorphous NiP/Hβ catalyst was prepared successfully further. Due to the superior surface property of amorphous NiP/Hβ catalyst, it exhibited good catalytic application for n-hexane isomerization. The catalytic activity of amorphous NiP/Hβ catalyst was close to that of the prepared Pt/Hβ sample, and better than that of commercial catalyst and crystalline Ni2P/Hβ catalyst. What's more, the amorphous NiP/Hβ catalyst shows high resistance to different sulfur compounds and water on account of its unique surface property. The effect of loading amounts on surface property and catalytic performance was investigated, and the structure-function relationship among them was studied ulteriorly. The results demonstrate that loading amounts have effect on textural property and surface acid property, which further affect the catalytic performance. The 10 wt.% NiP/Hβ sample has appropriate pore structure and acid property with uniformly dispersed NiP nanoparticles on surface, which is helpful for providing suitable synergistic effect. The effects of reaction conditions on surface reactions and the mechanism for n-hexane isomerization were investigated further. Based on these results, the amorphous NiP/Hβ catalyst with superior surface property probably pavesa way to overcome the drawbacks of traditional noble metal catalyst, which shows good catalytic application prospects.

  4. K (Na)-promoted Ni, Al layered double hydroxide catalysts for the steam reforming of methanol

    Science.gov (United States)

    Qi, Caixia; Amphlett, John C.; Peppley, Brant A.

    Production of hydrogen by methanol steam reforming has been studied over a series of Ni/Al layered double hydroxide catalysts prepared by the co-precipitation method, with the aim to develop a stable catalyst that can be used in a membrane-joint performer at temperatures greater than 300 °C. H 2, CO and CO 2 are generally the major products together with trace amounts of CH 4. The presence of potassium and/or sodium cations was found to improve the activity of methanol conversion. The selectivity for CO 2 rather than CO was better with K ions than Na ions, especially at higher temperatures (e.g. 390-400 °C). Methanol steam reforming over a K-promoted Ni/Al layered double hydroxide catalyst resulted in better activity and similar stability compared to a commercial Cu catalyst.

  5. Intermetallic compounds of Ni and Ga as catalysts for the synthesis of methanol

    DEFF Research Database (Denmark)

    Sharafutdinov, Irek; Elkjær, Christian Fink; de Carvalho, Hudson Wallace Pereira

    2014-01-01

    In this work, we present a detailed study of the formation of supported intermetallic Ni–Ga catalysts for CO2 hydrogenation to methanol. The bimetallic phase is formed during a temperature-programmed reduction of the metal nitrates. By utilizing a combination of characterization techniques...... demonstrate that the catalysts with the desired intermetallic phase and composition are formed upon reduction in hydrogen and enable us to propose a mechanism of the Ni–Ga nanoparticles formation. By studying the effect of calcination prior to catalyst reduction, we show that the reactivity depends......, in particular in situ and ex situ X-ray diffraction, in situ X-ray absorption spectroscopy, transmission electron microscopy combined with electron energy loss spectroscopy and X-ray fluorescence, we have studied the formation of intermetallic Ni–Ga catalysts of two compositions: NiGa and Ni5Ga3. These methods...

  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. Ni-P and Ni-Cu-P modified carbon catalysts for methanol electro-oxidation in KOH solution

    Energy Technology Data Exchange (ETDEWEB)

    Hameed, R.M. Abdel [Department of Chemistry, Faculty of Science, Cairo University, Giza (Egypt); El-Khatib, K.M. [Chem. Eng. and Pilot Plant Department Engineering Division, National Research center, Dokki, Giza (Egypt)

    2010-03-15

    The electrocatalytic oxidation of methanol was studied on Ni-P and Ni-Cu-P supported over commercial carbon electrodes in 0.1 M KOH solution. Cyclic voltammetry and chronoamperometry techniques were employed. Electroless deposition technique was adopted for the preparation of these catalysts. The effect of the electroless deposition parameters on the catalytic activity of the formed samples was examined. They involve the variation of the deposition time, pH and temperature. The scanning electron micrography showed a compact Ni-P surface with a smooth and low porous structure. A decreased amount of nickel and phosphorus was detected by EDX analysis in the formed catalyst after adding copper to the deposition solution. However, an improvement in the catalytic performance of Ni-Cu-P/C samples was noticed. This is attributed to the presence of copper hydroxide/nickel oxyhydroxide species. It suppresses the formation of {gamma}-NiOOH phase and stabilizes {beta}-NiOOH form. Linear dependence of the oxidation current density on the square root of the scan rate reveals the diffusion controlled behaviour. (author)

  8. Efficient Hydrogenolysis of Guaiacol over Highly Dispersed Ni/MCM-41 Catalyst Combined with HZSM-5

    Directory of Open Access Journals (Sweden)

    Songbai Qiu

    2016-09-01

    Full Text Available A series of MCM-41 supported Ni catalysts with high metal dispersion was successfully synthesized by simple co-impregnation using proper ethylene glycol (EG. The acquired Ni-based catalysts performed the outstanding hydrogenolysis activity of guaiacol. The effects of the synthesis parameters including drying temperature, calcination temperature, and metal loading on the physical properties of NiO nanoparticles were investigated through the use of X-ray diffraction (XRD. The drying temperature was found to significantly influence the particle sizes of NiO supported on MCM-41, but the calcination temperature and metal loading had less influence. Interestingly, the small particle size (≤3.3 nm and the high dispersion of NiO particles were also obtained for co-impregnation on the mixed support (MCM-41:HZSM-5 = 1:1, similar to that on the single MCM-41 support, leading to excellent hydrogenation activity at low temperature. The guaiacol conversion could reach 97.9% at 150 °C, and the catalytic activity was comparative with that of noble metal catalysts. The hydrodeoxygenation (HDO performance was also promoted by the introduction of acidic HZSM-5 zeolite and an 84.1% yield of cyclohexane at 240 °C was achieved. These findings demonstrate potential applications for the future in promoting and improving industrial catalyst performance.

  9. Hydrodeoxygenation of bio-oil using different mesoporous supports of NiMo catalysts

    Science.gov (United States)

    Rinaldi, Nino; Simanungkalit, Sabar P.; Kristiani, Anis

    2017-11-01

    Biomass as a renewable and sustainable resources need to utilize in many applications, especially for energy application. One of its energy application is about converting biomass into bio-oil. High oxygen content in bio-oil needs to be upgraded through hydrodeoxygenation process before being used as transportation fuel. The development of heterogenenous catalysts become an important aspect in hydrodeoxygenation process, in particular the upgrading process of bio-oil. Several supporting mesoporous materials, such as TiO2, Al2O3 and MCM-41 have unique properties, both physical and chemical properties that can be utilized in various application, including catalyst. These heterogeneous catalysts were modified their catalytic properties by impregnation with some transition metal. The effect of various supporting material and transition metal impregnated were also studied. Their chemical and physical properties were characterized by X-Ray Diffraction, X-Ray Fluororesence, Fourier Transform Infra-Red, and Surface Area Analyzer. The result of characterizations showed that Ni-Mo/TiO2 is more crystalline than Ni-Mo/MCM-41 and Ni-Mo/Al2O3. In other hand, the specific surface area of Ni-Mo/TiO2 is lower than others. These heterogeneous catalysts were tested their catalytic activity in upgrading bio-oil. The liquid products produced were analyzed by using Elemental Analyzer. The result of catalytic activity tests showed catalysts resulted Ni-Mo/TiO2 exhibits best catalytic activity in hydrodeoxygenation process. The oxygen content decreased significantly from 41.61% to 26.22% by using Ni-Mo/TiO2. Compared with Ni-Mo/TiO2, Ni-Mo/MCM-41 and Ni-Mo/Al2O3 decrease lower to 33.22% % and 28.34%, respectively. Ni-Mo/TiO2 also resulted the highest Deoxygenation Degree (DOD) as of 55% compared with Ni-Mo/MCM-41 and Ni-Mo/Al2O3 as of 31.99 % and 47.99%, respectively.

  10. Effect of preparation parameters on the microporous structure of Ni/SiO{sub 2} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Castillon, F.F.; Bodganchikova, N. [Centro de Investigacion Cientifica y de Educacion Superior, Ensenada (Mexico); Fuentes, S.; Avalos, M. [Univ. Nacional Autonoma de Mexico, Ensenada (Mexico). Inst. de Fisica

    1996-12-31

    In this work the authors report the synthesis of Ni/SiO{sub 2} catalysts promoted by group 2 (IIA) cations (calcium and barium) which are currently used as hydrogenation catalysts. The effect of the preparation parameters-aging, base agent, and type of cation, on the surface area of catalysts--is evaluated. Catalysts were prepared by precipitation of the precursor silicic acid, along with nickel nitrate and calcium and barium carbonates, with NaOH, NH{sub 4}OH and Na{sub 2}CO{sub 3} as precipitating agents. Catalysts were characterized by diffuse reflectance spectra (DRS) and by BET-surface area measurements. Results are discussed in terms of sol-gel chemistry.

  11. Catalytic performance of Ni/MgO catalyst in methane dry reforming

    Science.gov (United States)

    Al-Swai, Basem M.; Osman, N. B.; Abdullah, Bawadi

    2017-10-01

    Methane dry reforming to synthesis gas over nickel catalysts supported on magnesium oxide has been studied. The support was prepared via co-precipitation method using ammonia solution (20 wt% in water) as the precipitating agent. 10 wt% of Ni metal was impregnated to form Ni/MgO catalyst. The prepared catalyst was characterized by different techniques, such as XRD, BET, SEM, and TGA analysis. The effect of reaction conditions on the conversions of CH4 and CO2, selectivity of H2 and CO, and carbon deposition were investigated in a tabular furnace reactor. The catalyst afforded as high as 93% CH4 conversion at 900 °C. The catalyst has also shown excellent stability during reaction at relatively higher space velocity (1.8×104 ml g-1 h-1) and 800 °C reaction temperature. TGA characterization of spent catalyst has shown lesser magnitude of carbon deposition on the surface of the catalyst at 900 °C.

  12. Tuning the interface of Ni@Ni(OH)2/Pd/rGO catalyst to enhance hydrogen evolution activity and stability

    Science.gov (United States)

    Deng, Zihua; Wang, Jun; Nie, Yao; Wei, Zidong

    2017-06-01

    The interface engineering is vital to rational design and synthesis of the heterogeneous catalyst for high-performance electrochemically applications. The smart and elaborate architecture design offers several remarkable advantages, including good dispersion, more exposed active site and good electrical conductivity. We report a trace Pd induced formation of Ni@Ni(OH)2/Pd catalyst on reduced graphene oxides (rGO) by hydrothermal synthesis. We found that the presence of palladium seeds can promote the grain refinement and dispersion of the catalyst. The HRTEM results revealed that most of Ni@Ni(OH)2/Pd with a mean size of ∼10 nm are uniformly dispersed on the rGO sheets, with Pd particles and Ni@Ni(OH)2 balls located side by side. DFT calculations further confirmed a strong interaction existed in the interfaces, which leads to a stable Ni@Ni(OH)2/Pd/rGO morphology. By tailoring Ni@Ni(OH)2-Pd-rGO interfaces of the catalyst, the catalyst gives a current density of 10 mA cm-2 at a small over-potential of 76 mV and exhibits an excellent stability for the hydrogen evolution reaction in an alkaline environments.

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

    Directory of Open Access Journals (Sweden)

    Shouyun Cheng

    2017-04-01

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

  14. Steam reforming of biomass gasification tar using benzene as a model compound over various Ni supported metal oxide catalysts.

    Science.gov (United States)

    Park, Hyun Ju; Park, Sung Hoon; Sohn, Jung Min; Park, Junhong; Jeon, Jong-Ki; Kim, Seung-Soo; Park, Young-Kwon

    2010-01-01

    The steam reforming of benzene as a model compound of biomass gasification tar was carried out over various Ni/metal oxide catalysts. The effects of the support, temperature, Ni-precursor, Ni loading and reaction time were examined, and their catalytic performance was compared with that of a commercial Ni catalyst. Among the Ni/metal oxide catalysts used, 15 wt% Ni/CeO(2)(75%)-ZrO(2)(25%) showed the highest catalytic performance owing to its greater redox characteristics and increased surface area, irrespective of the reaction temperature. The catalytic activity of 15 wt% Ni/CeO(2)(75%)-ZrO(2)(25%) was higher than that of the commercial Ni catalyst. Moreover, the catalyst activity was retained due to its excellent resistance to coke deposition even after 5h. The Ni-precursor played a critical role in the catalytic activity. With the exception of nickel nitrate, all the Ni-precursors (chloride and sulfate) caused deactivation of the catalyst.

  15. Hydrogen Production via Glycerol Dry Reforming over La-Ni/Al2O3 Catalyst

    Directory of Open Access Journals (Sweden)

    Kah Weng Siew

    2013-12-01

    Full Text Available Glycerol (a bio-waste generated from biodiesel production has been touted as a promising bio-syngas precursor via reforming route. Previous studies have indicated that carbon deposition is the major performance-limiting factor for nickel (Ni catalyst during glycerol steam reforming. In the current paper, dry (CO2-reforming of glycerol, a new reforming route was carried out over alumina (Al2O3-supported non-promoted and lanthanum-promoted Ni catalysts. Both sets of catalysts were synthesized via wet co-impregnation procedure. The physicochemical characterization of the catalyst showed that the promoted catalyst possessed smaller metal crystallite size, hence higher metal dispersion compared to the virgin Ni/Al2O3 catalyst. This was also corroborated by the surface images captured by the FESEM analysis. In addition, BET surface area measurement gave 92.05m²/g for non-promoted Ni catalyst whilst promoted catalysts showed an average of 1 to 6% improvement depending on the La loading. Reaction studies at 873 K showed that glycerol dry reforming successfully produced H2 with glycerol conversion and H2 yield that peaked at 9.7% and 25% respectively over 2wt% La content. The optimum catalytic performance by 2%La-Ni/Al2O3 can be attributed to the larger BET surface area and smaller crystallite size that ensured accessibility of active catalytic sites.  © 2013 BCREC UNDIP. All rights reservedReceived: 12nd May 2013; Revised: 7th October 2013; Accepted: 16th October 2013[How to Cite: Siew, K.W., Lee, H.C., Gimbun, J., Cheng, C.K. (2013. Hydrogen Production via Glycerol Dry Reforming over La-Ni/Al2O3 Catalyst. Bulletin of Chemical Reaction Engineering & Catalysis, 8 (2: 160-166. (doi:10.9767/bcrec.8.2.4874.160-166][Permalink/DOI: http://dx.doi.org/10.9767/bcrec.8.2.4874.160-166

  16. Bimetallic Pt-Ni catalysts supported on usy zeolite for n-hexane isomerization

    Directory of Open Access Journals (Sweden)

    F. V. Barsi

    2009-06-01

    Full Text Available Isomerization of linear alkanes has had considerable importance for the refining industry because the isomers formed in this reaction have high octane number. Most works reported in the literature studied the use of bifunctional catalysts, i.e., ones that have acid sites and metallic sites. In this study, bifunctional monometallic (Ni or Pt and bimetallic catalysts (Pt-Ni, using HUSY zeolite as the support, were prepared in order to verify the role of the metal content and composition on the catalytic properties for n-hexane isomerization. The method used for metal dispersion in the zeolite was competitive ion exchange using ammine complexes [Ni(NH36]Cl2 and [Pt(NH34]Cl2 as precursors. Four series of catalysts with constant atomic metal content had total metal amounts between 130 and 280 µmol M/g cat. Catalysts were characterized by temperature programmed reduction (TPR and subjected to catalytic evaluation for n-hexane isomerization at 250 ºC and 1 atm using H2/C6 = 9 molar ratio. TPR results show an easier reducibility of Ni+2 cations in the presence of Pt, which was evidenced by the displacement of the reduction peak of those cations towards lower temperatures in bimetallic catalysts. The bimetallic catalysts presented a higher activity in the isomerization of n-hexane when compared to the monometallic ones, as well better stability as the Pt content in the solid increases. The results of the activity as a function of the Pt content in the bimetallic catalysts show a maximum value around 50% of Pt. An addition of Pt above this critical value leads to a small decrease of the catalytic activity.

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

    Directory of Open Access Journals (Sweden)

    Istadi Istadi

    2011-11-01

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

  18. A novel nano-Ni/SiO2 catalyst for hydrogen production from steam reforming of ethanol.

    Science.gov (United States)

    Wu, Chunfei; Williams, Paul T

    2010-08-01

    Catalytic steam reforming of ethanol has been regarded as a promising way to produce hydrogen. However, catalytic deactivation is a key problem in the process. In this paper, a novel nano-Ni/SiO2 catalyst was prepared by a simple sol-gel method and compared to catalysts prepared by an impregnation method in relation to the steam reforming ethanol process. Good Ni dispersion and high BET surface areas (>700 m2 g(-1)) were obtained for sol-gel catalysts, whereas only 1 m2 g(-1) surface area was obtained for the Ni/SiO2 impregnation catalyst. The results of catalytic steam reforming of ethanol showed that about twice of the hydrogen production was produced with the Ni/SiO2 catalyst prepared by sol-gel (around 0.2 g h(-1)) compared with that prepared by impregnation (around 0.1 g h(-1)). The analysis of the used catalysts showed that 10Ni/SiO2-B and 20Ni/SiO2-B presented the highest stability, while other catalysts were fragmented into small pieces after the reforming process, especially the catalysts prepared by impregnation. A novel catalyst has been produced that has been shown to be effective in the production of hydrogen from the steam reforming of ethanol.

  19. Evaluation of CO oxidation over Co3O4-supported NiO catalysts

    Science.gov (United States)

    Sie, Min-Chun; Jeng, Pei-Di; Chen, Pin-Hsuan; Wu, Ruei-Ci; Wang, Chen-Bin

    2017-09-01

    The process of doping NiO onto Co3O4 for achieving resistance to sintering and obtaining long-term stability of catalytic activity was examined herein. A sample of cobalt oxide (Co3O4) was prepared from Co(NO3)2.6H2O via precipitation by NaOH, and then calcined at 300 and 500 °C. The Co3O4-supported NiO catalysts were prepared by deposited precipitation of Ni(NO3)2.6H2O with NaOH added in a dropwise manner into the suspended Co3O4 solution with various loading of nickel. Then, oxidation with NaOCl was employed to obtain NiO/Co3O4 catalysts (weight loading of Ni: 0.1 ˜ 5 wt%). All of the samples were characterized by using XRD, SEM/TEM, BET, TPR and TGA techniques. Catalytic activities related to CO oxidation were tested from 0 to 200 °C in a self-designed fluidized micro-reactor. The results showed that the calcination temperature and loading of nickel were important parameters in the preparation process. With the lower calcined temperature and loading of nickel below 1 wt%, all the samples showed high initial catalytic activity for CO oxidation near room temperature. The synergistic effect can induce CO oxidation between NiO and Co3O4, and probably constitute a more suitable redox property for the 0.2%Ni/Co3O4 (C3) catalyst. Furthermore, only a slight decrease of CO conversion (less than 5%) was observed after 50 h of continuous reaction under 125 °C on this catalyst. The CO conversion could still remain above 75% after 50 h, which demonstrates that the 0.2%Ni/Co3O4 (C3) sample can function as a durable CO oxidation catalyst. We confirmed that our designed catalysts, based on tiny NiO nanoparticles, can be used as a component of a toxic gas abatement system.

  20. Preparation and characterization of NiW-nHA composite catalyst for hydrocracking

    Science.gov (United States)

    Zhou, Gang; Hou, Yongzhao; Liu, Lei; Liu, Hongru; Liu, Can; Liu, Jing; Qiao, Huiting; Liu, Wenyong; Fan, Yubo; Shen, Shituan; Rong, Long

    2012-11-01

    The synthesis, characterization and catalytic capability of the NiW-nano-hydroxyapatite (NiW-nHA) composite were investigated in this paper. The NiW-nHA catalyst was prepared by a co-precipitation method. Then Fourier transform infrared (FT-IR) spectroscopy, transmission electron microscopy (TEM), X-ray diffraction (XRD) and energy dispersive spectroscopy (EDX) were used to analyze this material. In addition, the catalytic capacity of the NiW-nHA composite was also examined by FT-IR and gas chromatography (GC). The results of FT-IR analysis indicated that Ni, W and nHA combined closely. TEM observation revealed that this catalyst was needle shaped and the crystal retained a nanometer size. XRD data also suggested that a new phase of CaWO4 appeared and the lattice parameters of nHA changed in this system. nHA was the carrier of metals. The rates of Ni/W-loading were 73.24% and 65.99% according to the EDX data, respectively. Furthermore, the conversion of 91.88% Jatropha oil was achieved at 360 °C and 3 MPa h-1 over NiW-nHA catalyst. The straight chain alkanes ranging from C15 to C18 were the main components in the production. The yield of C15-C18 alkanes was up to 83.56 wt%. The reaction pathway involved hydrocracking of the C&z.dbd;C bonds of these triglycerides from Jatropha oil. This paper developed a novel non-sulfided catalyst to obtain a ``green biofuel'' from vegetable oil.

  1. Photocatalytic Hydrogen Production using Polymeric Carbon Nitride with a Hydrogenase and a Bioinspired Synthetic Ni Catalyst**

    OpenAIRE

    Caputo, Christine Amanda; Gross, Manuela A.; Lau, Vincent W; Cavazza, Christine; Lotsch, Bettina V.; Reisner, Erwin

    2014-01-01

    Solar-light-driven H2 production in water with a [NiFeSe]-hydrogenase (H2ase) and a bioinspired synthetic nickel catalyst (NiP) in combination with a heptazine carbon nitride polymer, melon (CNx), is reported. The semibiological and purely synthetic systems show catalytic activity during solar light irradiation with turnover numbers (TONs) of more than 50 000 mol H2 (mol H2ase)?1 and approximately 155 mol H2 (mol NiP)?1 in redox-mediator-free aqueous solution at pH 6 and 4.5, respectively. Bo...

  2. Conversion of furan derivatives for preparation of biofuels over Ni-Cu/C catalyst

    DEFF Research Database (Denmark)

    Fu, Zhaolin; Wang, Z.; Lin, Weigang

    2017-01-01

    Conversions of furfural and 5-hydroxymethylfurfural as model components in bio-oil were investigated over Ni-Cu/C catalyst with formic acid as hydrogen donor in isopropanol solvent to produce biofuels. The effects of reaction temperature, feed ratio, and reaction time were studied. A high yield...... biofuels from furan derivatives....

  3. USE OF Ni-Co ALLOY AS CATHODE CATALYST IN SINGLE CHAMBER MICROBIAL FUEL CELL

    Directory of Open Access Journals (Sweden)

    Paweł Piotr Włodarczyk

    2017-04-01

    Full Text Available Technology of microbial fuel cells allowing for the direct production of electricity from biodegradable materials can provide only energy production, but also wastewater treatment. This technology is seen as supporting of the traditional wastewater treatment. One of the problems with microbial fuel cells is a low current density of those energy sources. Nonetheless, it is possible to increase the current density by using the catalyst for electrodes (anode and cathode. The possibility of wastewater treatment using the Ni-Co alloy as catalyst for single chamber microbial fuel cells is presented in this paper. The studies have included measurements of H2O2 reduction on Ni-Co catalyst, power of cell and current density and also COD reduction. The reduction time for COD with the use of single chamber microbial fuel cell with Ni-Co cathode is similar to the reduction time with aeration. In analysed cell was obtained cell power of 13 mW, and current density of 0.21 mA/cm2. The possibility of using the Ni-Co alloy as catalyst for cathode of single chamber microbial fuel cells is presented in this paper.

  4. 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)

  5. NiFe(C2O4)xas a heterogeneous Fenton catalyst for removal of methyl orange.

    Science.gov (United States)

    Liu, Yucan; Zhang, Guangming; Chong, Shan; Zhang, Nan; Chang, Huazhen; Huang, Ting; Fang, Shunyan

    2017-05-01

    This paper studies a heterogeneous Fenton catalyst NiFe(C 2 O 4 ) x , which showed better catalytic activity than Ni(C 2 O 4 ) x and better re-usability than Fe(C 2 O 4 ) x . The methyl orange removal efficiency was 98% in heterogeneous Fenton system using NiFe(C 2 O 4 ) x . The prepared NiFe(C 2 O 4 ) x had a laminated shape and the size was in the range of 2-4 μm, and Ni was doped into catalyst's structure successfully. The NiFe(C 2 O 4 ) x had a synergistic effect of catalyst of 24.7 for methyl orange removal, and the dope of Ni significantly reduced the leaching of Fe by 77%. The reaction factors and kinetics were investigated. Under the optimal conditions, 0.4 g/L of catalyst dose and 10 mmol/L of hydrogen peroxide concentration, 98% of methyl orange was removed within 20 min. Analysis showed that hydroxyl radicals and superoxide radicals participated in the reaction. With NiFe(C 2 O 4 ) x catalyst, the suitable pH range for heterogeneous Fenton system was wide from 3 to 10. The catalyst showed good efficiency after five times re-use. NiFe(C 2 O 4 ) x provided great potential in treatment of refractory wastewater with excellent property. Copyright © 2017 Elsevier Ltd. All rights reserved.

  6. The effect of precipitants on Ni-Al2O3 catalysts prepared by a co-precipitation method for internal reforming in molten carbonate fuel cells

    Science.gov (United States)

    Jung, You-Shick; Yoon, Wang-Lai; Seo, Yong-Seog; Rhee, Young-Woo

    2012-01-01

    Ni-Al2O3 catalysts are prepared via the co-precipitation method using various precipitants: urea, Na2CO3, NaOH, K2CO3, KOH and NH4OH. The effects of the precipitants on the physicochemical properties and catalytic activities of the Ni-Al2O3 catalysts are investigated. The Ni50-urea catalyst displays the largest specific surface area and the highest pore volume. This catalyst also exhibits the highest Ni dispersion and the largest Ni surface area. Ni50-urea catalyst prepared with urea as precipitant and Ni50-K2CO3 catalyst prepared with K2CO3 as precipitant exhibit high pore volumes and good catalytic activities for methane steam reforming. The Ni50-urea catalyst exhibits the best physicochemical properties and shows good catalytic activity and a strong resistance to electrolyte contamination. PMID:22962548

  7. Selective Ring Opening of 1-Methylnaphthalene Over NiW-Supported Catalyst Using Dealuminated Beta Zeolite.

    Science.gov (United States)

    Kim, Eun-Sang; Lee, You-Jin; Kim, Jeong-Rang; Kim, Joo-Wan; Kim, Tae-Wan; Chae, Ho-Jeong; Kim, Chul-Ung; Lee, Chang-Ha; Jeong, Soon-Yong

    2016-02-01

    Nanoporous Beta zeolite was dealuminated by weak acid treatment for reducing the acidity. Bi-functional catalysts were prepared using commercial Beta zeolites and the dealuminated zeolites for acidic function, NiW for metallic function. 1-Methylnaphthalene was selected as a model compound for multi-ring aromatics in heavy oil, and its selective ring opening reaction has been investigated using the prepared bi-functional catalysts with different acidity in fixed bed reaction system. The dealuminated Beta zeolites, which crystal structure and nanoporosity were maintained, showed the higher SiO2/Al2O3 ratio and smaller acidity than their original zeolite. NiW-supported catalyst using the dealuminated Beta zeolite with SiO2/Al203 mole ratio of 55 showed the highest performance for the selective ring opening. The acidity of catalyst seemed to play an important role as active sites for the selective ring opening of 1-methylnaphthalene but there should be some optimum catalyst acidity for the reaction. The acidity of Beta zeolite could be controlled by the acid treatment and the catalyst with the optimum acidity for the selective ring opening could be prepared.

  8. Transformation of Sodium Bicarbonate and CO2 into Sodium Formate over NiPd Nanoparticle Catalyst

    Directory of Open Access Journals (Sweden)

    Mengnan eWang

    2013-09-01

    Full Text Available The present research systematically investigated, for the first time, the transformation of sodium bicarbonate and CO2 into sodium formate over a series of Ni based metal nanoparticles (NPs. Ni NPs and eight NiM (M stands for a second metal NPs were prepared by a facile wet chemical process and then their catalytic performance were evaluated in sodium bicarbonate hydrogenation. Bimetallic NiPd NPs with a composition of 7:3 were found to be superior for this reaction, which are more active than both pure Ni and Pd NPs. Hot filtration experiment suggested the NPs to be the truly catalytic active species and kinetic analysis indicated the reaction mechanism to be different than most homogeneous catalysts. The enhanced activity of the bimetallic nanoparticles may be attributed to their smaller size and improved stability.

  9. Origin of low temperature deactivation of Ni5Ga3 nanoparticles as catalyst for methanol synthesis

    DEFF Research Database (Denmark)

    Gardini, Diego; Sharafutdinov, Irek; Damsgaard, Christian Danvad

    In an effort to find alternative energy sources capable to compete with fossil fuels, methanol synthesis could represent a realistic solution to store “green” hydrogen produced from electrolysis or photo-induced water splitting. Recently, density functional theory (DFT) calculations [1] proposed Ni......-Ga alloys as active catalysts for methanol production from syngas mixtures and Ni-Ga nanoparticles supported on highly porous silica have been prepared using an incipient wetness impregnation technique from a solution of nickel and gallium nitrates [2]. Tests conducted in a fixed-bed reactor showed...... that the highest methanol yield is obtained with a Ni5Ga3 alloy exposed to a 25% CO2 – 75% H2 reaction mixture at 210 °C [2]. Under these experimental conditions, the catalyst is found to lose 35% of its activity after 20 hours of continuous testing at both 1 and 5 Bars. Although in situ XRD and EXAFS studies [3...

  10. 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.

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

    Directory of Open Access Journals (Sweden)

    Josh Y.Z. Chiou

    2017-02-01

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

  12. PYROLYSIS OF BROWN COAL USING A CATALYST BASED ON W–Ni

    Directory of Open Access Journals (Sweden)

    Lenka Jílková

    2015-10-01

    Full Text Available Tars from pyrolysis of brown coal can be refined to obtain compounds suitable for fuel production. However, it is problematic to refine the liquids from brown coal pyrolysis, because high molecular compounds are produced, and the sample solidifies. Therefore we decided to investigate the possibility of treating the product in the gas phase during pyrolysis, using a catalyst. A two-step process was investigated: thermal-catalytic refining. In the first step, alumina was used as the filling material, and in the second step a catalyst based on W-Ni was used. These materials were placed in two separate layers above the coal, so the volatile products passed through the alumina and catalyst layers. Pyrolysis tests showed that using the catalyst has no significant effect on the mass balance, but it improves the properties of the gas and the properties of the organic part of the liquid pyrolysis products, which will then be processed further.

  13. Density functional theory study for the enhanced sulfur tolerance of Ni catalysts by surface alloying

    Science.gov (United States)

    Hwang, Bohyun; Kwon, Hyunguk; Ko, Jeonghyun; Kim, Byung-Kook; Han, Jeong Woo

    2018-01-01

    Sulfur compounds in fuels deactivate the surface of anode materials in solid oxide fuel cells (SOFCs), which adversely affect the long-term durability. To solve this issue, it is important to design new SOFC anode materials with high sulfur tolerance. Unfortunately, it is difficult to completely replace the traditional Ni anode owing to its outstanding reactivity with low cost. As an alternative, alloying Ni with transition metals is a practical strategy to enhance the sulfur resistance while taking advantage of Ni metal. Therefore, in this study, we examined the effects of transition metal (Cu, Rh, Pd, Ag, Pt, and Au) doping into a Ni catalyst on not only the adsorption of H2S, HS, S, and H but also H2S decomposition using density functional theory (DFT) calculations. The dopant metals were selected rationally by considering the stability of the Ni-based binary alloys. The interactions between sulfur atoms produced by H2S dissociation and the surface are weakened by the dopant metals at the topmost layer. In addition, the findings show that H2S dissociation can be suppressed by doping transition metals. It turns out that these effects are maximized in the Au-doped Ni catalyst. Our DFT results will provide useful insights into the design of sulfur-tolerant SOFC anode materials.

  14. Effects of impregnation methods and drying conditions on quinoline hydrodenitrogenation over Ni-W based catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Guo, Fang; Qiu, Zegang; Zhao, Liangfu; Xiang, Hongwei [Institute of Coal Chemistry, Chinese Academy of Sciences (China); Guo, Shaoqing [Taiyuan University of Science and Technology (China)

    2014-04-15

    The effects of impregnation methods (co-impregnation and sequential impregnation) and drying conditions (air and vacuum) on the structure and catalytic behavior of MCM-41 supported Ni-W catalysts were investigated. The catalysts were characterized by powder X-ray diffraction (XRD) analysis, Fourier-transform infrared spectroscopy (FT-IR), diffuse reflectance UV-Vis absorbance spectroscopy (DRS), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and pyridine adsorbed infrared spectroscopy (Py-IR) techniques. They were tested for hydrodenitrogenation (HDN) of quinoline at temperatures of 300-400 deg C. The HDN results showed that the catalysts prepared by co-impregnation were more active than the catalysts prepared by sequential impregnation and the catalysts prepared by drying under vacuum were more active than the catalysts dried in air. Characterization revealed that the co-impregnation method and drying under vacuum promoted the dispersion of W, the formation of the active phases, and the formation of acidic sites on the catalysts. (author)

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

    Directory of Open Access Journals (Sweden)

    Ezekiel Dixon Dikio

    2011-01-01

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

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

    Science.gov (United States)

    Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank; Elkjær, Christian F; Hummelshøj, Jens S; Dahl, Søren; Chorkendorff, Ib; Nørskov, Jens K

    2014-04-01

    The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni5Ga3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al2O3 catalysts revealed the same or better methanol synthesis activity, as well as considerably lower production of CO. We suggest that this is a first step towards the development of small-scale low-pressure devices for CO2 reduction to methanol.

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

    Science.gov (United States)

    Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank; Elkjær, Christian F.; Hummelshøj, Jens S.; Dahl, Søren; Chorkendorff, Ib; Nørskov, Jens K.

    2014-04-01

    The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni5Ga3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al2O3 catalysts revealed the same or better methanol synthesis activity, as well as considerably lower production of CO. We suggest that this is a first step towards the development of small-scale low-pressure devices for CO2 reduction to methanol.

  18. Effect of Ni-Co Ternary Molten Salt Catalysts on Coal Catalytic Pyrolysis Process

    Science.gov (United States)

    Cui, Xin; Qi, Cong; Li, Liang; Li, Yimin; Li, Song

    2017-08-01

    In order to facilitate efficient and clean utilization of coal, a series of Ni-Co ternary molten salt crystals are explored and the catalytic pyrolysis mechanism of Datong coal is investigated. The reaction mechanisms of coal are achieved by thermal gravimetric analyzer (TGA), and a reactive kinetic model is constructed. The microcosmic structure and macerals are observed by scanning electron microscope (SEM). The catalytic effects of ternary molten salt crystals at different stages of pyrolysis are analyzed. The experimental results show that Ni-Co ternary molten salt catalysts have the capability to bring down activation energy required by pyrolytic reactions at its initial phase. Also, the catalysts exert a preferable catalytic action on macromolecular structure decomposition and free radical polycondensation reactions. Furthermore, the high-temperature condensation polymerization is driven to decompose further with a faster reaction rate by the additions of Ni-Co ternary molten salt crystal catalysts. According to pyrolysis kinetic research, the addition of catalysts can effectively decrease the activation energy needed in each phase of pyrolysis reaction.

  19. Steam reforming of ethanol over Ni-based catalysts: Effect of feed composition on catalyst stability

    DEFF Research Database (Denmark)

    Trane-Restrup, Rasmus; Dahl, Søren; Jensen, Anker Degn

    2014-01-01

    In this work the effects of steam-to-carbon ratio (S/C), and addition of H2 or O2 to the feed on the product yields and carbon deposition in the steam reforming (SR) of ethanol over Ni/MgAl2O4, Ni/Ce0.6Zr0.4O2, and Ni/CeO2 at 600 °C have been investigated. Increasing the S/C-ratio from 1.6 to 8.3...

  20. O-Carboxymethyl Chitosan Supported Heterogeneous Palladium and Ni Catalysts for Heck Reaction

    Directory of Open Access Journals (Sweden)

    Dongjun Lv

    2017-01-01

    Full Text Available Two polymer catalysts (Pd-OCMCS and Ni-OCMCS with good reusability were synthesized by coordinating Pd and Ni onto O-carboxymethyl chitosan (OCMCS. The chemical structure and thermal stability of prepared catalysts were determined by Fourier transform infrared (FT-IR spectra, Energy Dispersive Spectrometer (EDSanalysis, X-ray diffraction (XRD, and thermogravimetric analyzer (TG-DTG, and the analysis results showed that the Pd and Ni ions coordinated onto the OCMCS and formed a ligand with the –COOH group, amino groups, and –OH group on the OCMCS, and the EDS and Inductively Coupled Plasma Optical Emission Spectrometry (ICP-OES analysis results showed that the loading amounts of Pd and Ni were approximately 8.3% and 8.9%, respectively. In the Heck reaction between aryl halides and n-butyl acrylate catalyzed by the prepared catalyst, the test results showed that the product yield followed the order of aryl iodide > aryl bromide > aryl chloride. Additionally, the product yield for the aryl iodide and aryl bromide could reach up to 99% and 96%, respectively. Moreover, the electron-withdrawing and electron-donating property of the group on the aryl also affected the product yield, and the product yield for aryl halides with electron-withdrawing group p-NO2, p-CH3CO, and p-CHO was higher than that with electron-donating group p-CH3.

  1. Synergism between unsupported Re and Co or Ni sulfide catalysts in the HDS and HDN of gas oil

    Energy Technology Data Exchange (ETDEWEB)

    Escalona, N.; Garcia, R. [Facultad de Ciencias Quimicas, Universidad de Concepcion, Concepcion (Chile); Ojeda, J.; Baeza, P.; Gil-Llambas, F.J. [Universidad de Santiago de Chile, Casilla 40, Correo 33, Santiago (Chile); Palacios, J.M.; Fierro, J.L.G.; Agudo, A. Lopez [Instituto de Catalisis y Petroleoquimica, CSIC, Cantoblanco, 28049, Madrid (Spain)

    2005-06-15

    Two series of unsupported Co-Re and Ni-Re binary sulfide catalysts with variable atomic ratio {alpha}=Me/(Me+Re) from 0 to 1 were prepared by the co-maceration method. The catalysts were characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), and evaluated in the simultaneous hydrodesulfurization (HDS) and hydrodenitrogenation (HDN) reactions of a real gas oil feed under industrial relevant conditions. The results showed a synergetic effect of the Co or Ni sulfide on the ReS{sub 2} in both HDS and HDN reactions. A maximum in activity at the same atomic ratio {alpha} circa 0.5 was observed for both reactions and both Co-Re and Ni-Re catalysts. The magnitude of the synergy was generally superior for HDS than for HDN, and at low reaction temperature (598K) larger for Ni-Re than for Co-Re catalysts, especially in HDS, while at high temperature (648K) it was reverse. Moreover, the Co-Re catalysts exhibited higher HDN/HDS selectivity than the Ni-Re catalysts. Neither XRD nor XPS results evidenced the presence of a Co-Re-S or Ni-Re-S like phase. It is suggested that the synergism could be associated to the hydrogen activation and spillover from the Co or Ni sulfide to ReS{sub 2}.

  2. Raney-platinum film electrodes for potentially implantable glucose fuel cells. Part 1: Nickel-free glucose oxidation anodes

    Energy Technology Data Exchange (ETDEWEB)

    Kerzenmacher, S.; von Stetten, F. [Laboratory for MEMS Applications, Department of Microsystems Engineering- IMTEK, University of Freiburg, Georges-Koehler-Allee 106, 79110 Freiburg (Germany); Schroeder, M. [Institut fuer Anorganische und Analytische Chemie, University of Freiburg, Albertstrasse 21, 79104 Freiburg (Germany); Braemer, R. [Hochschule Offenburg- University of Applied Sciences, Badstrasse 24, 79652 Offenburg (Germany); Zengerle, R. [Laboratory for MEMS Applications, Department of Microsystems Engineering- IMTEK, University of Freiburg, Georges-Koehler-Allee 106, 79110 Freiburg (Germany); Centre for Biological Signalling Studies (bioss), Albert-Ludwigs-Universitaet Freiburg (Germany)

    2010-10-01

    We present a novel fabrication route yielding Raney-platinum film electrodes intended as glucose oxidation anodes for potentially implantable fuel cells. Fabrication roots on thermal alloying of an extractable metal with bulk platinum at 200 C for 48 h. In contrast to earlier works using carcinogenic nickel, we employ zinc as potentially biocompatible alloying partner. Microstructure analysis indicates that after removal of extractable zinc the porous Raney-platinum film (roughness factor {proportional_to}2700) consists predominantly of the Pt{sub 3}Zn phase. Release of zinc during electrode operation can be expected to have no significant effect on physiological normal levels in blood and serum, which promises good biocompatibility. In contrast to previous anodes based on hydrogel-bound catalyst particles the novel anodes exhibit excellent resistance against hydrolytic and oxidative attack. Furthermore, they exhibit significantly lower polarization with up to approximately 100 mV more negative electrode potentials in the current density range relevant for fuel cell operation. The anodes' amenability to surface modification with protective polymers is demonstrated by the exemplary application of an approximately 300 nm thin Nafion coating. This had only a marginal effect on the anode long-term stability and amino acid tolerance. While in physiological glucose solution after approximately 100 h of operation gradually increasing performance degradation occurs, rapid electrode polarization within 24 h is observed in artificial tissue fluid. Optimization approaches may include catalyst enhancement by adatom surface modification and the application of specifically designed protective polymers with controlled charge and mesh size. (author)

  3. Lanthanum and cerium co-modified Ni/SiO2 catalyst for CO methanation from syngas

    Science.gov (United States)

    Gong, Dandan; Li, Shuangshuang; Guo, Shaoxia; Tang, Honggui; Wang, Hong; Liu, Yuan

    2018-03-01

    Sintering of active metal nanoparticles (NPs) and carbon deposition is critical problems for many metal catalysts, such as nickel based catalysts for generating methane from syngas. To improve the resistance to the sintering and carbon deposition, a new scheme was proposed in this work. Lanthanum and cerium co-modified Ni/SiO2 catalysts were synthesized by using perovskite type oxide of La1-xCexNiO3 loaded on SiO2 as the precursor. In a nanocrystallite of La1-xCexNiO3, ions of nickel, lanthanum and cerium are evenly mixed at atomic level and confined in the nanocrystallite, therefore, Ni NPs and the two promoters of La2O3 and CeO2 should be in close contact and highly dispersed on SiO2 after reduction. The catalysts were characterized by using XRD, TEM, BET, H2-TPD, XPS, TG and Raman techniques. Compared with the mono-promoted catalysts, the bi-promoted La0.75Ce0.25NiO3/SiO2 showed much better resistance to carbon deposition, higher resistance to sintering and higher activity for CO methanation, which are attributed to co-eliminating effect of the two promoters for the deposited carbon, confinement of the interacted two promoters for Ni NPs and the higher dispersion of Ni NPs derived from the smaller size of La0.75Ce0.25NiO3.

  4. Ni/Mo2C nanowires and their carbon-coated composites as efficient catalysts for nitroarenes hydrogenation

    Science.gov (United States)

    Shu, Yijin; He, Sina; Xie, Lifang; Chan, Hang Cheong; Yu, Xiang; Yang, Lichun; Gao, Qingsheng

    2017-02-01

    The hydrogenation of nitroarenes to value-added aromatic amines requires active and selective catalysts. Due to the good efficiency, economic cost and high earth-abundance, Ni-based nanostructures emerge as the promising catalysts, which are however limited by the poor dispersion and unsatisfied durability. Herein, Mo2C nanowires was introduced as a versatile support towards the highly dispersive Ni owing to the strong metal-support interactions on carbide surface, accomplishing the high activity in the hydrogenation of 3-nitrobenzoic acid, 4-nitrobenzoic acid and nitrobenzene. However, the presence of water that promoted the selective hydrogenation unfortunately deactivated Ni species. An effective carbon coating was further introduced to remarkably enhance the stability, protecting active Ni from corrosive H+ and H2O. This work elucidates a feasible way towards efficient and stable catalysts by the introduction of both carbide supports and carbon coating, shedding some light on the development of high-performance catalysts.

  5. Study of structural and catalytic properties of Ni catalysts prepared from inorganic complex precursor for Fischer-Tropsch synthesis

    Science.gov (United States)

    Saheli, Sania; Rezvani, Ali Reza; Malekzadeh, Azim

    2017-09-01

    The silica- and alumina- supported Ni catalysts synthesized by thermal decomposition of inorganic precursors were evaluated for Fischer-Tropsch synthesis (FTS); the structural properties and performance of the catalysts were compared to those of samples constructed via impregnation method. The results revealed that the synthesized catalysts have higher catalytic activity comparison to those prepared via the conventional impregnation method. The effect of the preparation method on the structural properties shows that synthesizing the catalyst through inorganic precursor route is more appropriate. Characterization of catalysts is carried out using inductively coupled plasma (ICP), powder X-ray diffraction (XRD), scanning electron microscopy (SEM), and BET specific surface area.

  6. Ni-Based Catalysts for Low Temperature Methane Steam Reforming: Recent Results on Ni-Au and Comparison with Other Bi-Metallic Systems

    Directory of Open Access Journals (Sweden)

    Anna M. Venezia

    2013-06-01

    Full Text Available Steam reforming of light hydrocarbons provides a promising method for hydrogen production. Ni-based catalysts are so far the best and the most commonly used catalysts for steam reforming because of their acceptably high activity and significantly lower cost in comparison with alternative precious metal-based catalysts. However, nickel catalysts are susceptible to deactivation from the deposition of carbon, even when operating at steam-to-carbon ratios predicted to be thermodynamically outside of the carbon-forming regime. Reactivity and deactivation by carbon formation can be tuned by modifying Ni surfaces with a second metal, such as Au through alloy formation. In the present review, we summarize the very recent progress in the design, synthesis, and characterization of supported bimetallic Ni-based catalysts for steam reforming. The progress in the modification of Ni with noble metals (such as Au and Ag is discussed in terms of preparation, characterization and pretreatment methods. Moreover, the comparison with the effects of other metals (such as Sn, Cu, Co, Mo, Fe, Gd and B is addressed. The differences of catalytic activity, thermal stability and carbon species between bimetallic and monometallic Ni-based catalysts are also briefly shown.

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

    Directory of Open Access Journals (Sweden)

    Yanyan Feng

    2015-01-01

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

  8. A Ni(iii) complex stabilized by silica nanoparticles as an efficient nanoheterogeneous catalyst for oxidative C-H fluoroalkylation.

    Science.gov (United States)

    Khrizanforov, Mikhail N; Fedorenko, Svetlana V; Strekalova, Sofia O; Kholin, Kirill V; Mustafina, Asiya R; Zhilkin, Mikhail Ye; Khrizanforova, Vera V; Osin, Yuri N; Salnikov, Vadim V; Gryaznova, Tatyana V; Budnikova, Yulia H

    2016-07-26

    We have developed Ni(III)-doped silica nanoparticles ([(bpy)xNi(III)]@SiO2) as a recyclable, low-leaching, and efficient oxidative functionalization nanocatalyst for aromatic C-H bonds. The catalyst is obtained by doping the complex [(bpy)3Ni(II)] on silica nanoparticles along with its subsequent electrooxidation to [(bpy)xNi(III)] without an additional oxidant. The coupling reaction of arenes with perfluoroheptanoic acid occurs with 100% conversion of reactants in a single step at room temperature under nanoheterogeneous conditions. The catalyst content is only 1% with respect to the substrates under electrochemical regeneration conditions. The catalyst can be easily separated from the reaction mixture and reused a minimum of five times. The results emphasize immobilization on the silica support and the electrochemical regeneration of Ni(III) complexes as a facile route for developing an efficient nanocatalyst for oxidative functionalization.

  9. Study of NiMoS mixed phase from catalyst precursors in residue slurry-bed hydrocracking

    Science.gov (United States)

    Du, Juntao; Deng, Wenan; Li, Chuan; Zhang, Zailong; Sun, Qiang; Cao, Xiangpeng; Yang, Tengfei

    2017-03-01

    The evolution and role of NiMoS structures from catalyst precursors on residue hydrocracking was investigated. NiMoS mixed phase played important roles in unsupported catalyst and heavy oil development, such as synergy effect and coke inhibiting. The oil-soluble molybdenum naphthenate and nickel naphthenate were chosen as catalyst precursors. The mixtures of the precursor were compared to those of other monometallic oil-soluble precursor in an effort to evaluate the evolution and role of NiMoS phase in the slurry bed hydrocracking of heavy oil. The presence of NiMoS phase were characterized by X-ray diffraction (XRD), TEM and XPS. The series of tests in the slurry-phase reactor was to confirm the synergy effect of NiMoS mixed phase.

  10. Impact of heating rate and solvent on Ni-based catalysts prepared by solution combustion method for syngas methanation

    Directory of Open Access Journals (Sweden)

    Zeng Yan

    2014-12-01

    Full Text Available Ni-Al2O3 catalysts prepared by solution combustion method for syngas methanation were enhanced by employing various heating rate and different solvent. The catalytic properties were tested in syngas methanation. The result indicates that both of heating rate and solvent remarkably affect Ni particle size, which is a key factor to the catalytic activity of Ni-Al2O3 catalysts for syngas methanation. Moreover, the relationship between Ni particle size and the production rate of methane per unit mass was correlated. The optimal Ni-Al2O3 catalyst prepared in ethanol at 2°C/min, achieves a maximum production rate of methane at the mean size of 20.8 nm.

  11. Catalyst for the manufacture of gases containing methane. [Al-Ni compounds

    Energy Technology Data Exchange (ETDEWEB)

    Broecker, F.J.; Zirker, G.; Triebskorn, B.; Marosi, L.; Schwarzmann, M.; Dethlefsen, W.; Kaempfer, K.

    1973-11-13

    A catalyst is produced by the process consisting essentially of precipitating the compound Ni/sub 6/Al/sub 2/(OH)/sub 16/.CO/sub 3/.4H/sub 2/O as a catalyst precursor from an aqueous medium; drying said precipitate at a temperature of from 80 to 180/sup 0/C; raising the temperature of said precipitate between the drying stage and the calcination stage at a gradient of 1.66/sup 0/C/minute to 3.3/sup 0/C/minute; calcining said precipitate at a temperature of from 300 to 550/sup 0/C; and thereafter reducing said precipitate in a stream of hydrogen to form said catalyst.

  12. Deactivating Carbon Formation on a Ni/Al2O3 Catalyst under Methanation Conditions

    DEFF Research Database (Denmark)

    Olesen, Sine Ellemann; Andersson, Klas J.; Damsgaard, Christian Danvad

    2017-01-01

    The carbon formation causing deactivation during CO methanation was studied for a Ni/Al2O3 catalyst. Sulfur-free methanation at low temperature (573 K) for various lengths of time was followed by temperature-programmed hydrogenation (TPH) providing information on carbon types involved in the deac......The carbon formation causing deactivation during CO methanation was studied for a Ni/Al2O3 catalyst. Sulfur-free methanation at low temperature (573 K) for various lengths of time was followed by temperature-programmed hydrogenation (TPH) providing information on carbon types involved...... in the deactivation of the catalyst.Three main carbon hydrogenation peaks were evident from TPHs following methanation: ∼460, ∼650, and ∼775 K. It is suggested that the ∼460 K TPH peak was composed of two peaks: a surface carbide peak at 445–460 K, and a peak due to carbon dissolved into the nickel at 485 K based...... on CO and CH4 adsorption measurements and XRD analysis. The 650 and 775 K temperature peaks are assigned to polymerized carbon structures and the ∼775K peak was found to be the primary cause of deactivation as judged by a linear correlation between its amount and the degree of catalyst deactivation...

  13. Hydrocracking of Jatropha Oil over non-sulfided PTA-NiMo/ZSM-5 Catalyst

    Science.gov (United States)

    Yang, Xiaosong; Liu, Jing; Fan, Kai; Rong, Long

    2017-01-01

    The PTA-NiMo/ZSM-5 catalyst impregnated with phosphotungstic acid (PTA) was designed for the transformation of Jatropha oil into benzene, toluene, and xylenes (BTX) aromatics. The produced catalyst was characterized by N2 adsorption-desorption, powder X-ray diffraction (XRD), Fourier transform infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), and the temperature-programmed desorption of ammonia (NH3-TPD). The catalytic performance was evaluated by gas chromatography (GC). The liquid products were 70 wt% of the feed oil, and the majority of the liquid products were BTX. The aromatization activity of the catalyst was improved by the addition of PTA and the hierarchical process. The favorable PTA amount was 20 wt% and the yield of BTX was 59 wt% at 380 °C, 3 MPa, H2/oil (v/v) = 1000 and LHSV = 1 h−1 over the PTA20-NiMo/HZ0.5 catalyst (PTA 20 wt%) without sulfurization. PMID:28134313

  14. Synergetic effects leading to coke-resistant NiCo bimetallic catalysts for dry reforming of methane

    KAUST Repository

    Li, Lidong

    2015-01-08

    A new dry reforming of methane catalyst comprised of NiCo bimetallic nanoparticles and a Mgx(Al)O support that exhibits high coke resistance and long-term on-stream stability is reported. The structural characterization by XRD, TEM, temperature-programmed reduction, and BET analysis demonstrates that the excellent performance of this catalyst is ascribed to the synergy of various parameters, including metal-nanoparticle size, metal-support interaction, catalyst structure, ensemble size, and alloy effects.

  15. In situ growth of carbon nanotubes on Ni/MgO: a facile preparation of efficient catalysts for the production of synthetic natural gas from syngas.

    Science.gov (United States)

    Fan, M T; Lin, J D; Zhang, H B; Liao, D W

    2015-11-07

    Ni/MgO-CNTs catalysts are prepared by in situ chemical vapor deposition growth of CNTs on Ni/MgO. These catalysts exhibit an improved performance for the production of synthetic natural gas from syngas, which is attributed to the formation of highly catalytic active interfaces among Ni, CNTs and MgO.

  16. Hydrocracking of Cerbera manghas Oil with Co-Ni/HZSM-5 as Double Promoted Catalyst

    Directory of Open Access Journals (Sweden)

    Lenny Marlinda

    2017-05-01

    Full Text Available The effect of various reaction temperature on the hydrocracking of Cerbera manghas oil to produce a paraffin-rich mixture of hydrocarbons with Co-Ni/HZSM-5 as doubled promoted catalyst were studied. The Co-Ni/HZSM-5 catalyst with various metal loading and metal ratio was prepared by incipient wetness impregnation. The catalysts were characterized by XRD, AAS, and N2 adsorption-desorption. Surface area, pore diameter, and pore volume of catalysts decreased with the increasing of metals loading. The hydrocracking process was conducted under hydrogen initial pressure in batch reactor equipped with a mechanical stirrer. The reaction was carried out at a temperature of 300-375 oC for 2 h.  Depending on the experimental condition, the reaction pressure changed between 10 bar and 15 bar.   Several parameters were used to evaluate biofuel produced, including oxygen removal, hydrocarbon composition and gasoline/kerosene/diesel yields. Biofuel was analyzed by Fourier Transform Infrared Spectroscopic (FTIR and gas chromatography-mass spectrometry (GC-MS. The composition of hydrocarbon compounds in liquid products was similar to the compounds in the gasoil sold in unit of Pertamina Gas Stations, namely pentadecane, hexadecane, heptadecane, octadecane, and nonadecane with different amounts for each biofuel produced at different reaction temperatures. However, isoparaffin compounds were not formed at all operating conditions. Pentadecane (n-C15 and heptadecane (n-C17 were the most abundant composition in gasoil when Co-Ni/HZSM-5 catalyst was used. Cerbera Manghas oil can be recommended as the source of non-edible vegetable oil to produce gasoil as an environmentally friendly transportation fuel. Copyright © 2017 BCREC Group. All rights reserved Received: 20th May 2016; Revised: 30th January 2017; Accepted: 10th February 2017 How to Cite: Marlinda, L., Al-Muttaqii, M., Gunardi, I., Roesyadi, A., Prajitno, D.H. (2017. Hydrocracking of Cerbera manghas Oil

  17. Ni-Supported Pd Nanoparticles with Ca Promoter: A New Catalyst for Low-Temperature Ammonia Cracking.

    Directory of Open Access Journals (Sweden)

    Jaroslaw Polanski

    Full Text Available In this paper we report a new nanometallic, self-activating catalyst, namely, Ni-supported Pd nanoparticles (PdNPs/Ni for low temperature ammonia cracking, which was prepared using a novel approach involving the transfer of nanoparticles from the intermediate carrier, i.e. nano-spherical SiO2, to the target carrier technical grade Ni (t-Ni or high purity Ni (p-Ni grains. The method that was developed allows a uniform nanoparticle size distribution (4,4±0.8 nm to be obtained. Unexpectedly, the t-Ni-supported Pd NPs, which seemed to have a surface Ca impurity, appeared to be more active than the Ca-free (p-Ni system. A comparison of the novel PdNPs/Ni catalyst with these reported in the literature clearly indicates the much better hydrogen productivity of the new system, which seems to be a highly efficient, flexible and durable catalyst for gas-phase heterogeneous ammonia cracking in which the TOF reaches a value of 2615 mmolH2/gPd min (10,570 molNH3/molPd(NP h at 600°C under a flow of 12 dm3/h (t-Ni.

  18. A possible highly active supported Ni dimer catalyst for O{sub 2} dissociation: A first-principles study

    Energy Technology Data Exchange (ETDEWEB)

    Dong, Shan [College of Physics and Materials Science, Henan Normal University, Xinxiang, Henan 453007 (China); Zhang, Yanxing, E-mail: 2016025@htu.edu.cn [College of Physics and Materials Science, Henan Normal University, Xinxiang, Henan 453007 (China); Zhang, Xilin; Mao, Jianjun [College of Physics and Materials Science, Henan Normal University, Xinxiang, Henan 453007 (China); Yang, Zongxian, E-mail: yzx@henannu.edu.cn [College of Physics and Materials Science, Henan Normal University, Xinxiang, Henan 453007 (China); Collaborative Innovation Center of Nano Functional Materials and Applications, Henan Province (China)

    2017-04-30

    Graphical abstract: The minimum energy paths (MEPs) for the dissociation process of O{sub 2} on the surfaces of bare YSZ (111) and Ni{sub n}/YSZ (111) (n = 1, 2 and 3). - Highlights: • The catalytic activity of supported metal catalysts is closely related to the size of metal particles. • The dissociation of O{sub 2} on the YSZ (111) surface is largely enhanced by the supported Ni cluster. • The supported Ni dimer is predicted to be the smallest Ni cluster needed for efficient O{sub 2} dissociation. • The results would provide an important reference to improve the activity and efficiency of the Ni/YSZ(111) nanocomposite catalysts in cost-effective materials. - Abstract: The adsorption and dissociation of O{sub 2} on the supported small nickel clusters with one-, two-, three-Ni atoms on yttria-stabilized zirconia (YSZ) (111) surfaces, as well as those on the bare YSZ(111) and Ni(111) surfaces are comparatively studied using ab initio density functional theory calculations. It is found that the dissociation of O{sub 2} on the YSZ(111) surface is largely enhanced by the supported Ni dimer, which is predicted to be the smallest Ni cluster needed for efficient O{sub 2} dissociation. The results would provide an important reference to improve the activity and efficiency of the Ni/YSZ(111) nanocomposite catalysts in cost-effective materials.

  19. Electroless Deposition of Ni-P Alloys on Cenospheres by Using Silver as the Catalyst

    Science.gov (United States)

    Xu, Jian; Xiong, Weihao; Zeng, Aixiang

    Electroless deposition of Ni-P alloys on cenospheres is demonstrated in the present investigation. AgNO3 is used as an activator to replace the conventional PdCl2 activator and H2 PO-2 in the coating bath is used as the reducing agent to replace Sn2+ in order to lower the overall cost of the coating process. The coated cenospheres are characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDX) and powder X-ray diffraction (XRD). It shows that Ni-P alloys uniformly deposit on the surface of the cenospheres under experimental conditions. The possible mechanism of electroless Ni-P alloys coating of cenospheres by using silver as the catalyst is suggested.

  20. Green synthesis of Ni-Nb oxide catalysts for low-temperature oxidative dehydrogenation of ethane

    KAUST Repository

    Zhu, Haibo

    2015-03-05

    The straightforward solid-state grinding of a mixture of Ni nitrate and Nb oxalate crystals led to, after mild calcination (T<400°C), nanostructured Ni-Nb oxide composites. These new materials efficiently catalyzed the oxidative dehydrogenation (ODH) of ethane to ethylene at a relatively low temperature (T<300°C). These catalysts appear to be much more stable than the corresponding composites prepared by other chemical methods; more than 90% of their original intrinsic activity was retained after 50h with time on-stream. Furthermore, the stability was much less affected by the Nb content than in composites prepared by classical "wet" syntheses. These materials, obtained in a solvent-free way, are thus promising green and sustainable alternatives to the current Ni-Nb candidates for the low-temperature ODH of ethane.

  1. Characterization of Pt/HUSY and Pt-Ni/HUSY catalysts by transmission electron microscopy

    Directory of Open Access Journals (Sweden)

    Maura H. Jordão

    1999-07-01

    Full Text Available Bifunctional catalysts formed by metals (nickel, platinum as well as an association of both metals supported in an ultrastabilized Y molecular sieve (USY were prepared. The samples were obtained using a competitive ion exchange method, followed by calcination and reduction of the transition metal under hydrogen atmosphere. The solids were characterized by ICP for their chemical composition, XRD, TEM and the catalytic properties evaluated in the isomerization of the n-hexane. It was observed that the NH4USY zeolite support presented better ion exchange efficiency in comparison to that of the zeolite HUSY, due to the decrease of the pH of the reaction medium in the last case. The TEM images of the catalysts, obtained in both bright and dark field, showed that the metal particles are dispersed almost inside the molecular sieve micro and mesopores. TEM images of the catalysts obtained in bright field showed that the average particle diameter were 64 and 108 Å for platinum and nickel respectively and about 70 Å when both metals are present. In the mentioned reaction, platinum catalysts were more active and stable than the nickel ones and the catalysts formed by both metals (0,2%Pt + 0,8% Ni/HUSY presented the highest activity.

  2. Degradation of aniline by heterogeneous Fenton's reaction using a Ni-Fe oxalate complex catalyst.

    Science.gov (United States)

    Liu, Yucan; Zhang, Guangming; Fang, Shunyan; Chong, Shan; Zhu, Jia

    2016-11-01

    A Ni-Fe oxalate complex catalyst was synthesized and characterized by means of Brunauer-Emmet-Teller (BET) method, scanning electron microscope (SEM) and X-ray photo-electron spectroscopy (XPS). The catalyst showed good catalytic activity for aniline degradation by heterogeneous Fenton's reaction, in which the synergetic index was 9.3. The effects of reaction temperature, catalyst dosage, hydrogen peroxide concentration and initial pH were investigated. Under the optimum conditions (T = 293 K, catalyst dosage = 0.2 g/L, H2O2 concentration = 4 mmol/L and initial pH = 5.4), 100% aniline could be removed within 35 min, and approximately 88% deamination efficiency was achieved in 60 min. The aniline degradation process followed the pseudo-first-order kinetic (k = 0.177 min(-1)) with activation energy (Ea) of 49.4 kJ mol(-1). Aniline could be removed in a broad initial pH (3-8) due to the excellent pH-tolerance property of the catalyst. The detected ammonium ion indicated that deamination occurred during aniline degradation. It was proposed that deamination synchronized with aniline removal, and aniline was attacked by free radicals to generate benzoquinonimine and phenol. This system is promising for the removal of aniline from water. Copyright © 2016 Elsevier Ltd. All rights reserved.

  3. Orange Peel Oxidative Gasification on Ni Catalysts Promoted with CaO, CeO2 or K2O.

    Science.gov (United States)

    Vargas, G; Zapata, B; Valenzuela, M A; Alfaro, S

    2015-09-01

    Orange peel can be considered as an attractive raw material to be gasified for hydrogen or syngas production. In this work, the catalytic evaluation of several silica-supported nickel catalysts in the oxidative degradation of waste orange peel is reported. It was found that the catalytic gasification with the K2O-Ni/silica catalyst produces more hydrogen than the non-catalytic route at 600 degrees C. Surprisingly, a significant amount of ethene was obtained with the CeO2-Ni/silica catalyst, which was explained in terms of an oxidative dehydrogenation reaction of ethane formed during biomass or tar decomposition.

  4. CuNi NPs supported on MIL-101 as highly active catalysts for the hydrolysis of ammonia borane

    Science.gov (United States)

    Gao, Doudou; Zhang, Yuhong; Zhou, Liqun; Yang, Kunzhou

    2018-01-01

    The catalysts containing Cu, Ni bi-metallic nanoparticles were successfully synthesized by in-situ reduction of Cu2+ and Ni2+ salts into the highly porous and hydrothermally stable metal-organic framework MIL-101 via a simple liquid impregnation method. When the total amount of loading metal is 3 × 10-4 mol, Cu2Ni1@MIL-101 catalyst shows higher catalytic activity comparing to CuxNiy@MIL-101 with different molar ratio of Cu and Ni (x, y = 0, 0.5, 1.5, 2, 2.5, 3). Cu2Ni1@MIL-101 catalyst has the highest catalytic activity comparing to mono-metallic Cu and Ni counterparts and pure bi-metallic CuNi nanoparticles in hydrolytic dehydrogeneration of ammonia borane (AB) at room temperature. Additionally, in the hydrolysis reaction, the Cu2Ni1@MIL- 101 catalyst possesses excellent catalytic performances, which exhibit highly catalytic activity with turn over frequency (TOF) value of 20.9 mol H2 min-1 Cu mol-1 and a very low activation energy value of 32.2 kJ mol-1. The excellent catalytic activity has been successfully achieved thanks to the strong bi-metallic synergistic effects, uniform distribution of nanoparticles and the bi-functional effects between CuNi nanoparticles and the host of MIL-101. Moreover, the catalyst also displays satisfied durable stability after five cycles for the hydrolytically releasing H2 from AB. The non-noble metal catalysts have broad prospects for commercial applications in the field of hydrogen-stored materials due to the low prices and excellent catalytic activity.

  5. Formation of Multiple-Phase Catalysts for the Hydrogen Storage of Mg Nanoparticles by Adding Flowerlike NiS.

    Science.gov (United States)

    Xie, Xiubo; Ma, Xiujuan; Liu, Peng; Shang, Jiaxiang; Li, Xingguo; Liu, Tong

    2017-02-22

    In order to enhance the hydrogen storage properties of Mg, flowerlike NiS particles have been successfully prepared by solvothermal reaction method, and are subsequently ball milled with Mg nanoparticles (NPs) to fabricate Mg-5 wt % NiS nanocomposite. The nanocomposite displays Mg/NiS core/shell structure. The NiS shell decomposes into Ni, MgS and Mg2Ni multiple-phases, decorating on the surface of the Mg NPs after the first hydrogen absorption and desorption cycle at 673 K. The Mg-MgS-Mg2Ni-Ni nanocomposite shows enhanced hydrogenation and dehydrogenation rates: it can quickly uptake 3.5 wt % H2 within 10 min at 423 K and release 3.1 wt % H2 within 10 min at 573 K. The apparent hydrogen absorption and desorption activation energies are decreased to 45.45 and 64.71 kJ mol(-1). The enhanced sorption kinetics of the nanocomposite is attributed to the synergistic catalytic effects of the in situ formed MgS, Ni and Mg2Ni multiple-phase catalysts during the hydrogenation/dehydrogenation process, the porthole effects for the volume expansion and microstrain of the phase transformation of Mg2Ni and Mg2NiH4 and the reduced hydrogen diffusion distance caused by nanosized Mg. This novel method of in situ producing multiple-phase catalysts gives a new horizon for designing high performance hydrogen storage material.

  6. TiO{sub 2} nanotubes promoted PT-NI/C catalyst with low PT content as anode catalyst for direct ethanol fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Shen, L.; Jiang, Q.Z.; Gan, T.G.; Ma, Z.F. [Shanghai Jiao Tong Univ., Shanghai (China). Dept. of Chemical Engineering; Shen, M. [Oklahoma Univ., Norman, OK (United States). School of Chemical, Biological and Materials Engineering, Sarkeys Energy Center; Rodriguez Varela, F.J. [Cinvestav Unidad Saltillo, Coahuila (Mexico). Grupo de Recursos Naturales y Energeticos; Ocampo, A.L. [Univ. Nacional Autonoma, Mexico City (Mexico). Dept. de Quimica Analitica

    2010-07-15

    Although direct ethanol fuel cells (DEFC) have more energy density than direct methanol fuel cells (DMFC), their widespread use has been hampered by the fact that metallic platinum (Pt) catalysts are readily poisoned by strongly absorbed reaction intermediates such as CO{sub ads} at low operating temperatures. The addition of a second transition metal or a metal oxide component has been considered as a means to improve performance of DEFCs by forming a binary anode based on Pt. In this study, titanium oxide (TiO{sub 2}) nanotubes (TiO{sub 2}NTs) were added into a low-platinum content Pt-Ni/C catalyst to improve its catalytic activity for the ethanol oxidation reaction (EOR). The promotion effect of TiO{sub 2}NTs on Pt-Ni/C catalyst was examined. Cyclic voltametry (CV) and chronoamperometry showed that TiO{sub 2}NTs can improve the catalytic activity of the Pt-Ni/C catalyst considerably. Compared to a commercial Pt-Ru/C catalyst, the Pt-Ni-TiO{sub 2}NT/C catalyst has a larger electrochemical active surface (EAS) and has lower onset potential for the EOR. The elemental composition and electronic structure of the catalyst were characterized by X-ray photoelectron spectroscopy, energy dispersive X-ray spectrometry, inductively coupled plasma-optical emission spectrometry and X-ray diffraction. High resolution transmission electron microscopy was used to characterize the morphological properties of these catalysts. The study showed that onset oxidation potential can be lowered by the presence of TiO{sub 2}NTs because they retain more of the Pt metallic species and provide more hydroxides groups. 35 refs., 2 tabs., 10 figs.

  7. Raney-platinum film electrodes for potentially implantable glucose fuel cells. Part 2: Glucose-tolerant oxygen reduction cathodes

    Energy Technology Data Exchange (ETDEWEB)

    Kerzenmacher, S.; Kraeling, U.; von Stetten, F. [Laboratory for MEMS Applications, Department of Microsystems Engineering - IMTEK, University of Freiburg, Georges-Koehler-Allee 106, 79110 Freiburg (Germany); Schroeder, M. [Institut fuer Anorganische und Analytische Chemie, University of Freiburg, Albertstrasse 21, 79104 Freiburg (Germany); Braemer, R. [Hochschule Offenburg - University of Applied Sciences, Badstrasse 24, 79652 Offenburg (Germany); Zengerle, R. [Laboratory for MEMS Applications, Department of Microsystems Engineering - IMTEK, University of Freiburg, Georges-Koehler-Allee 106, 79110 Freiburg (Germany); Centre for Biological Signalling Studies (bioss), Albert-Ludwigs-Universitaet Freiburg (Germany)

    2010-10-01

    We report the fabrication and characterization of glucose-tolerant Raney-platinum cathodes for oxygen reduction in potentially implantable glucose fuel. Fabricated by extraction of aluminum from 1 {mu}m thin platinum-aluminum bi-layers annealed at 300 C, the novel cathodes show excellent resistance against hydrolytic and oxidative attack. This renders them superior over previous cathodes fabricated from hydrogel-bound catalyst particles. Annealing times of 60, 120, and 240 min result in approximately 400-550 nm thin porous films (roughness factors {proportional_to}100-150), which contain platinum and aluminum in a ratio of {proportional_to}9:1. Aluminum release during electrode operation can be expected to have no significant effect on physiological normal levels, which promises good biocompatibility. Annealing time has a distinct influence on the density of trenches formed in the cathode. Higher trench densities lead to lower electrode potentials in the presence of glucose. This suggests that glucose sensitivity is governed by mixed potential formation resulting from oxygen depletion within the trenches. During performance characterization the diffusion resistance to be expected from tissue capsule formation upon electrode implantation was taken into account by placing a membrane in front of the cathode. Despite the resulting limited oxygen supply, cathodes prepared by annealing for 60 min show more positive electrode potentials than previous cathodes fabricated from hydrogel-bound activated carbon. Compared to operation in phosphate buffered saline containing 3.0 mM glucose, a potential loss of approximately 120 mV occurs in artificial tissue fluid. This can be reduced to approximately 90 mV with a protective Nafion layer that is easily electro-coated onto the Raney-platinum film. (author)

  8. Application of Cement Clinker as Ni-Catalyst Support for Glycerol Dry Reforming

    Directory of Open Access Journals (Sweden)

    Hua Chyn Lee

    2013-12-01

    Full Text Available The increase in biodiesel production inevitably yield plethora of glycerol. Therefore, glycerol has been touted as the most promising source for bio-syngas (mixture of H2 and CO production. Significantly, coking on nickel-based catalysts has been identified as a major deactivation factor in reforming technology. Indeed, coke-resistant catalyst development is essential to enhance syngas production. The current work develops cement clinker (comprised of 62.0% calcium oxide-supported nickel catalyst (with metal loadings of 5, 10, 15 and 20 wt% for glycerol dry reforming (CO2. Physicochemical characterization of the catalysts was performed using XRD, XRF, BET, TGA and FESEM-EDS techniques. Subsequently, reaction studies were conducted in a 7-mm ID fixed-bed stainless steel reactor at 1023 K with various CO2 partial pressures at constant weight-hourly space velocity (WHSV of 7.2×104 ml gcat-1 h-1. Gas compositions were determined using Agilent 3000 micro-gas chromatography (GC and Lancom III gas analyzer. Results obtained showed an increment of BET surface area up to 32-fold with Ni loading which was corroborated by FESEM images. Syngas (H2 and CO ratios of less than 2 were being produced at 1023 K. A closer scrutiny to the transient profile revealed that the presence of CO2 higher or lower than CGR 1:1 promotes the Boudouard reaction. © 2013 BCREC UNDIP. All rights reservedReceived: 30th May 2013; Revised: 27th August 2013; Accepted: 11st September 2013[How to Cite: Lee, H.C., Siew, W.K., Cheng, C.K. (2013. Preparation Application of Cement Clinker as Ni-Catalyst Support for Glycerol Dry Reforming. Bulletin of Chemical Reaction Engineering & Catalysis, 8 (2: 137-144. (doi:10.9767/bcrec.8.2.5023.137-144][Permalink/DOI: http://dx.doi.org/10.9767/bcrec.8.2.5023.137-144

  9. 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.

  10. Recovery of Co, Ni, Mo, and V from unroasted spent hydrorefining catalysts by selective chlorination

    Energy Technology Data Exchange (ETDEWEB)

    Gaballah, I.; Djona, M. (Inst. National Polytechnique de Lorraine, Vandoeuvre (France))

    1995-02-01

    Spent hydrorefining catalysts may contain 4 to 6% of CoO and/or NiO, 8 to 16% of MoO[sub 3], and up to 10% of V[sub 2]O[sub 5], generally supported by alumina. They also contain up to 25% of carbon, hydrocarbons, and sulfur. Selective chlorination of raw, unroasted samples with Cl[sub 2] + air, Cl[sub 2] + N[sub 2], and Cl[sub 2] + CO + N[sub 2] gas mixtures have been investigated for the recovery of valuable elements. The fastest chlorination kinetics are obtained using the Cl[sub 2] + CO + N[sub 2] gas mixture, followed by Cl[sub 2] + N[sub 2]. The best selective chlorination of spent hydrorefining catalysts is obtained using a Cl[sub 2] + air gas mixture. At temperatures lower than 600 C, it is possible to recover more than 90% of the Ni and Co, about 99% of the Mo, and up to 75% of the V compounds. Cobalt and Nickel chlorides are extracted from the chlorination residues by their dissolution with water. Molybdenum and vanadium chlorides and/or oxychlorides are recovered by selective condensation from the vapor phase. The chlorination of the catalyst support, Al[sub 2]O[sub 3], can be limited to less than about 6%. A flow sheet is proposed.

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

    Science.gov (United States)

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

    2017-06-01

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

  12. Highly stable ceria-zirconia-yttria supported Ni catalysts for syngas production by CO2 reforming of methane

    Science.gov (United States)

    Muñoz, M. A.; Calvino, J. J.; Rodríguez-Izquierdo, J. M.; Blanco, G.; Arias, D. C.; Pérez-Omil, J. A.; Hernández-Garrido, J. C.; González-Leal, J. M.; Cauqui, M. A.; Yeste, M. P.

    2017-12-01

    Ni/CeO2/YSZ and Ni/Ce0.15Zr0.85O2 have been investigated as catalysts for the dry reforming of methane at 750 °C. Ni was incorporated by the impregnation method. The supports were previously activated by using a thermo-chemical protocol consisting on a severe reduction (H2/Ar) at 950 °C followed by a mild oxidation (O2/He) at 500 °C. According to TPR results, this protocol leads to the development of unique redox properties in the case of the CeO2/YSZ oxide. Two types of CO2 + CH4 (1:1) mixtures (helium-diluted and undiluted) were used to feed the reactor. When using the Ni/Ce0.15Zr0.85O2 catalyst with undiluted feed, the reactor became plugged by coke. By contrast, Ni/CeO2/YSZ behaved as an active and stable catalyst even under the most severe operation conditions. The characterization of the spent Ni/CeO2/YSZ using TGA, TEM, Raman and XPS spectroscopy revealed that only a limited amount of graphitic carbon, in form of nanotubes, was formed. No evidences of deactivating carbonaceous forms were obtained. The singular redox properties of the activated CeO2/YSZ oxides are proposed as a key for designing Ni catalysts highly stable in reforming processes.

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

    Directory of Open Access Journals (Sweden)

    Mérel Philippe

    2010-01-01

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

  14. Strategies for improving the performance and stability of Ni-based catalysts for reforming reactions.

    Science.gov (United States)

    Li, Shuirong; Gong, Jinlong

    2014-11-07

    Owing to the considerable publicity that has been given to petroleum related economic, environmental, and political problems, renewed attention has been focused on the development of highly efficient and stable catalytic materials for the production of chemical/fuel from renewable resources. Supported nickel nanoclusters are widely used for catalytic reforming reactions, which are key processes for generating synthetic gas and/or hydrogen. New challenges were brought out by the extension of feedstock from hydrocarbons to oxygenates derivable from biomass, which could minimize the environmental impact of carbonaceous fuels and allow a smooth transition from fossil fuels to a sustainable energy economy. This tutorial review describes the recent efforts made toward the development of nickel-based catalysts for the production of hydrogen from oxygenated hydrocarbons via steam reforming reactions. In general, three challenges facing the design of Ni catalysts should be addressed. Nickel nanoclusters are apt to sinter under catalytic reforming conditions of high temperatures and in the presence of steam. Severe carbon deposition could also be observed on the catalyst if the surface carbon species adsorbed on metal surface are not removed in time. Additionally, the production of hydrogen rich gas with a low concentration of CO is a challenge using nickel catalysts, which are not so active in the water gas shift reaction. Accordingly, three strategies were presented to address these challenges. First, the methodologies for the preparation of highly dispersed nickel catalysts with strong metal-support interaction were discussed. A second approach-the promotion in the mobility of the surface oxygen-is favored for the yield of desired products while promoting the removal of surface carbon deposition. Finally, the process intensification via the in situ absorption of CO2 could produce a hydrogen rich gas with low CO concentration. These approaches could also guide the design

  15. A one-dimensional porous carbon-supported Ni/Mo2C dual catalyst for efficient water splitting.

    Science.gov (United States)

    Yu, Zi-You; Duan, Yu; Gao, Min-Rui; Lang, Chao-Chao; Zheng, Ya-Rong; Yu, Shu-Hong

    2017-02-01

    The development of active, stable and low-cost electrocatalysts towards both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) for overall water splitting remains a big challenge. Herein, we report a new porous carbon-supported Ni/Mo2C (Ni/Mo2C-PC) composite catalyst derived by thermal treatment of nickel molybdate nanorods coated with polydopamine, which efficiently and robustly catalyses the HER and OER with striking kinetic metrics in alkaline electrolyte. The catalyst affords low onset potentials of -60 mV for the HER and 270 mV for the OER, as well as small overpotentials of 179 mV for the HER and 368 mV for the OER at a current density of 10 mA cm-2. These results compare favorably to Mo2C-PC, Ni-PC, and most other documented Ni- and Mo-based catalysts. The high activity of Ni/Mo2C-PC is likely due to electron transfer from Ni to Mo2C, leading to a higher Ni valence and a lower Mo valence in the Ni/Mo2C-PC catalyst, as these are HER and OER active species and thus account for the enhanced activity. Remarkably, our home-made alkaline electrolyser, assembled with Ni/Mo2C-PC as a bifunctional catalyst, can enable a water-splitting current density of 10 mA cm-2 to be achieved at a low cell voltage of 1.66 V.

  16. Effect of Ca, Ce or K oxide addition on the activity of Ni/SiO{sub 2} catalysts for the methane decomposition reaction

    Energy Technology Data Exchange (ETDEWEB)

    Zapata, Beatriz; Torres-Garcia, Enelio [Instituto Mexicano del Petroleo, Programa de Procesos y Reactores, Eje C. 152, Mexico, D.F., C.P. 07730 (Mexico); Valenzuela, Miguel A.; Palacios, Jorge [Instituto Politecnico Nacional-ESIQIE, Lab. Catalisis y Materiales, Zacatenco, Mexico, D.F., C.P. 07738 (Mexico)

    2010-11-15

    To increase the activity and stability of Ni/SiO{sub 2} catalysts, a series of Ni-Ca, Ni-K and Ni-Ce promoted catalysts were prepared by successive impregnations. The textural properties, reducibility and catalytic performance in the methane decomposition reaction were investigated. The catalyst containing 30 wt.% Ni and 30 wt.% cerium oxide greatly increased the conversion of methane (90% of equilibrium value) and improved the stability, whereas the Ni-K and Ni-Ca were less active and stable than the Ni/SiO{sub 2} catalyst. The results suggest that Ce addition prevents the sintering of nickel particles during reduction process maintaining a random distribution between the silica and cerium oxide improving the distribution and migration of deposited carbon. (author)

  17. 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

  18. Multifunctional Pd/Ni-Co catalyst for hydrogen production by chemical looping coupled with steam reforming of acetic acid.

    Science.gov (United States)

    Fermoso, Javier; Gil, María V; Rubiera, Fernando; Chen, De

    2014-11-01

    High yield of high-purity H2 from acetic acid, a model compound of bio-oil obtained from the fast pyrolysis of biomass, was produced by sorption-enhanced steam reforming (SESR). An oxygen carrier was introduced into a chemical loop (CL) coupled to the cyclical SESR process to supply heat in situ for the endothermic sorbent regeneration to increase the energy efficiency of the process. A new multifunctional 1 %Pd/20 %Ni-20 %Co catalyst was developed for use both as oxygen carrier in the CL and as reforming catalyst in the SESR whereas a CaO-based material was used as CO2 sorbent. In the sorbent-air regeneration step, the Ni-Co atoms in the catalyst undergo strong exothermic oxidation reactions that provide heat for the CaO decarbonation. The addition of Pd to the Ni-Co catalyst makes the catalyst active throughout the whole SESR-CL cycle. Pd significantly promotes the reduction of Ni-Co oxides to metallic Ni-Co during the reforming stage, which avoids the need for a reduction step after regeneration. H2 yield above 90 % and H2 purity above 99.2 vol % were obtained. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  19. Catalytic Chemical Vapor Deposition of Methane to Carbon Nanotubes: Copper Promoted Effect of Ni/MgO Catalysts

    Directory of Open Access Journals (Sweden)

    Wen Yang

    2014-01-01

    Full Text Available The Ni/MgO and Ni-Cu/MgO catalysts were prepared by sol-gel method and used as the catalysts for synthesis of carbon nanotubes by thermal chemical vapor deposition. The effect of Cu on the carbon yield and structure was investigated, and the effects of calcination temperature and reaction temperature were also investigated. The catalysts and synthesized carbon materials were characterized by temperature programmed reduction (TPR, thermogravimetric analysis (TGA, and scanning electron microscopy (SEM. Results showed that the addition of Cu promoted the reduction of nickel species, subsequently improving the growth and yield of CNTs. Meanwhile, CNTs were synthesized by the Ni/MgO and Ni-Cu/MgO catalysts with various calcination temperatures and reaction temperatures, and results suggested that the obtained CNTs on Ni-Cu/MgO catalyst with the calcination temperature of 500°C and the reaction temperature of 650°C were of the greatest yield and quantity of 927%.

  20. 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.

  1. 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.

  2. Efficient Water Electrolysis Using Ni2P as a Bifunctional Catalyst: Unveiling the Oxygen Evolution Catalytic Properties of Ni2P.

    Science.gov (United States)

    Stern, Lucas-Alexandre; Hu, Xile

    2016-01-01

    The excellent bifunctional catalytic activity of nickel phosphide (Ni2P) for water splitting is reported. Ni2P, an active hydrogen evolving catalyst, is shown to be highly active for oxygen evolution. Only 290 mV of overpotential is required to generate a current density of 10 mA cm(-2) in 1 M KOH. Under oxygen evolving conditions, Ni2P undergoes structural modification to form a Ni2P/NiOx core-shell assembly, the catalytic active species. Ni2P is applied on both electrodes of an alkaline electrolyser and a current density of 10 mA cm(-2) is generated at 1.63 V.

  3. Ni-Mn based alloys as versatile catalyst for different electrochemical reactions

    Science.gov (United States)

    Aaboubi, Omar; Ali-Omar, Ahmed-Yassin; Dzoyem, Eunice; Marthe, Jimmy; Boudifa, Mohamed

    2014-12-01

    To develop large scale use of hydrogen and fuel cells as a renewable energy source it is need to increase their durability and reduce their cost mainly due to the use of precious metals. We have examined new type of the low cost binary nickel-manganese (Ni-Mn) catalysts electrodeposited from ammonium chloride bath onto copper substrates. By varying bath composition, polarization potential and essentially bath temperature the operating deposition conditions were optimized to produce Ni-Mn coatings with high active surface (e.g. spongy aspect). The outstanding catalytic activity, the durability and the versatility of the deposited films have been characterized in basic media using several electrochemical processes, such as hydrogen evolution reaction (HER), water oxidation reaction (OER) and ethanol oxidation reaction (EOR).

  4. Enhanced carbon tolerance on Ni-based reforming catalyst with Ir alloying: A DFT study

    Science.gov (United States)

    Ahn, Kiyong; Choi, Sungjun; Lee, Jong-Ho; Kim, Byung-Kook; Kim, Jedo; Kim, Hyoungchul

    2017-10-01

    Carbon deposition is a major cause of performance degradation for the Ni-based catalyst used in steam reforming of hydrocarbons. In this work, we perform first principle calculations to show that carbon tolerance behavior can be significantly enhanced by alloying Ni with Ir. The most stable atomic structure predicted by the surface phased diagram shows that Ir atoms prefer to stay on the surface of the alloy ensuring their exposure to the incoming gas. We find that the presence of Ir atoms suppress the surface migration of carbon atoms and weaken the stability of the adsorbed carbon agglomerates. Finally, we elucidate that the local reactivity change caused by the shift in the d-band structure is responsible for such good carbon tolerance behavior.

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

    Science.gov (United States)

    Jung, Won Suk

    2018-03-15

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

  6. SHS-produced intermetallides as catalysts for hydrocarbons synthesis from CO and H{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Eliseev, O.L.; Kazantsev, R.V.; Davydov, P.E.; Lapidus, A.L. [Russian Academy of Sciences, Moscow (Russian Federation). N.D. Zelinsky Institute of Organic Chemistry; Borshch, V.N.; Pugacheva, E.V. [Russian Academy of Sciences, Chernogolovka (Russian Federation). Inst. of Structural Macrokinetics and Materials Science

    2012-07-01

    Raney-type polymetallic alloys were prepared by Self-Propagating High-Temperature Synthesis followed by alkaline treating. Surface morphology and composition of were studied using XRD, BET, SEM and EMPA techniques. The samples were tested in Fischer-Tropsch synthesis demonstrated rather high activity and very high selectivity to heavy paraffins. High selectivity to C{sub 5+} hydrocarbons is attributed to high thermal conductivity of alloys which prevents hot spots formation and therefore suppresses formation of methane and light hydrocarbons. Selectivity can be further improved by adding some d-metals in catalyst composition. Promotion with La seems to be particularly suitable for lowering methane formation while doping with Ni enhances methane yield greatly. (orig.)

  7. Selective hydrogenation of acetylene on SiO{sub 2} supported Ni-In bimetallic catalysts: Promotional effect of In

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Yanjun; Chen, Jixiang, E-mail: jxchen@tju.edu.cn

    2016-11-30

    Graphical abstract: A suitable Ni/In ratio remarkably enhanced the acetylene conversion, the selectivity to ethylene and the catalyst stability. Display Omitted - Highlights: • There was a promotional effect of In on the performance of Ni/SiO{sub 2}. • A suitable Ni/In ratio was required for good performance of Ni{sub x}In/SiO{sub 2}. • Both geometrical and electronic effects of In contributed to good performance. • Ni/SiO{sub 2} deactivation is mainly owing to phase change from Ni to nickel carbide. • The carbonaceous deposit was the main reason for Ni{sub x}In/SiO{sub 2} deactivation. - Abstract: Ni/SiO{sub 2} and the bimetallic Ni{sub x}In/SiO{sub 2} catalysts with different Ni/In ratios were tested for the selective hydrogenation of acetylene, and their physicochemical properties before and after the reaction were characterized by means of N{sub 2}-sorption, H{sub 2}-TPR, XRD, TEM, XPS, H{sub 2} chemisorption, C{sub 2}H{sub 4}-TPD, NH{sub 3}-TPD, FT-IR of adsorbed pyridine, and TG/DTA and Raman. A promotional effect of In on the performance of Ni/SiO{sub 2} was found, and Ni{sub x}In/SiO{sub 2} with a suitable Ni/In ratio gave much higher acetylene conversion, ethylene selectivity and catalyst stability than Ni/SiO{sub 2}. This is ascribed to the geometrical isolation of the reactive Ni atoms with the inert In ones and the charge transfer from the In atoms to Ni ones, both of which are favorable for reducing the adsorption strength of ethylene and restraining the C−C hydrogenolysis and the polymerizations of acetylene and the intermediate compounds. On the whole, Ni{sub 6}In/SiO{sub 2} and Ni{sub 10}In/SiO{sub 2} had better performance. Nevertheless, with increasing the In content, the selectivity to the C4+ hydrocarbons tended to increase due to the enhanced catalyst acidity because of the charge transfer from the In atoms to Ni ones. As the Lewis acid ones, the In sites could promote the polymerization. The catalyst deactivation was also analyzed

  8. An effective Pd-Ni(2)P/C anode catalyst for direct formic acid fuel cells.

    Science.gov (United States)

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

    2014-01-03

    The direct formic acid fuel cell is an emerging energy conversion device for which palladium is considered as the state-of-the-art anode catalyst. In this communication, we show that the activity and stability of palladium for formic acid oxidation can be significantly enhanced using nickel phosphide (Ni(2)P) nanoparticles as a cocatalyst. X-ray photoelectron spectroscopy (XPS) reveals a strong electronic interaction between Ni(2)P and Pd. A direct formic acid fuel cell incorporating the best Pd–Ni(2)P anode catalyst exhibits a power density of 550 mWcm(-2), which is 3.5 times of that of an analogous device using a commercial Pd anode catalyst.

  9. The effect of poly-N-vinylpyrrolidone modification on NiCoB catalysts for hydrogenation of p-chloronitrobenzene

    Energy Technology Data Exchange (ETDEWEB)

    Zhao Bin [Department of Chemical Engineering, Nanocatalysis Research Center, National Central University, Chung-Li 320, Taiwan (China); Chen Yuwen, E-mail: ywchen@cc.ncu.edu.tw [Department of Chemical Engineering, Nanocatalysis Research Center, National Central University, Chung-Li 320, Taiwan (China)

    2011-02-15

    A series of poly-N-vinylpyrrolidone (PVP)-modified NiCoB catalysts with various PVP contents were prepared by chemical reduction method. The Ni and Co cations were reduced by NaBH{sub 4} at room temperature. PVP was added during preparation. The materials were characterized by X-ray diffraction, transmission electron microscopy, and differential scanning calorimeter. The results showed that all samples possessed amorphous structure. After washing, the residual PVP adsorbed on the surface of NiCoB and acted as a spacer to prevent NiCoB particles from aggregation and agglomeration. The liquid-phase hydrogenation of p-chloronitrobenzene was carried out to investigate the catalytic properties of the PVP-modified NiCoB catalysts. The catalytic activities of NiCoB catalysts decreased by modifying with PVP but the selectivities for p-chloroaniline improved significantly. The competitive adsorption of PVP with p-chloronitrobenzene and p-chloroaniline on the NiCoB nanoparticles was responsible for the catalytic performance. The amount of the PVP played a key role in the hydrogenation reaction.

  10. Highly active Ni/Y-doped ZrO{sub 2} catalysts for CO{sub 2} methanation

    Energy Technology Data Exchange (ETDEWEB)

    Takano, H., E-mail: takano_hi@hitachizosen.co.jp [Hitachi Zosen Corporation, Kashiwa, 277-8515 (Japan); Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo, 060-8628 (Japan); Kirihata, Y.; Izumiya, K.; Kumagai, N. [Hitachi Zosen Corporation, Kashiwa, 277-8515 (Japan); Habazaki, H., E-mail: habazaki@eng.hokudai.ac.jp [Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo, 060-8628 (Japan); Division of Applied Chemistry & Frontier Chemistry Center, Faculty of Engineering, Hokkaido University, Sapporo, 060-8628 (Japan); Hashimoto, K. [Tohoku Institute of Technology, Sendai, 277-8515 (Japan)

    2016-12-01

    Highlights: • The Ni/Y-doped ZrO{sub 2} catalysts show highly catalytic activity for CO{sub 2} methanation. • Bidentate carbonate is a major adsorption spice on the Ni/Y-doped ZrO{sub 2} catalysts. • The oxide support of t-ZrO{sub 2} and/or c-ZrO{sub 2} with oxygen vacancies plays a key role. - Abstract: The catalytic methanation of CO{sub 2} was carried out on Ni catalysts supported on Y-doped ZrO{sub 2} with various Y{sup 3+} concentrations and Ni/(Zr + Y) molar ratio = 1. The catalysts were characterized by X-ray diffraction, scanning transmission electron microscopy, specific surface area, temperature-programmed desorption of CO{sub 2}, and temperature-programmed reaction. In addition, operando diffuse-reflectance infrared Fourier-transform spectroscopy (DRIFT) was used to identify the adsorbed reaction intermediate. Catalysts supported on Y-doped ZrO{sub 2} show higher catalytic activity than the catalyst on Y-free ZrO{sub 2} with a monoclinic ZrO{sub 2} phase. The catalytic activity is also dependent upon the Y{sup 3+} concentration, and the highest activity was obtained for the catalyst with a Y/(Zr + Y) molar ratio of 0.333, which consists mainly of fcc Ni and cubic ZrO{sub 2} phase. Y{sup 3+} doping into ZrO{sub 2} introduces oxygen vacancies, which play an important role in enhancing the catalytic activity. The operando DRIFT study reveals that a CO adsorption intermediate is absent, and bidentate carbonate is an important intermediate for CH{sub 4} formation.

  11. Formation and Yield of Multi-Walled Carbon Nanotubes Synthesized via Chemical Vapour Deposition Routes Using Different Metal-Based Catalysts of FeCoNiAl, CoNiAl and FeNiAl-LDH

    Directory of Open Access Journals (Sweden)

    Mohd Zobir Hussein

    2014-11-01

    Full Text Available Multi-walled carbon nanotubes (MWCNTs were prepared via chemical vapor deposition (CVD using a series of different catalysts, derived from FeCoNiAl, CoNiAl and FeNiAl layered double hydroxides (LDHs. Catalyst-active particles were obtained by calcination of LDHs at 800 °C for 5 h. Nitrogen and hexane were used as the carrier gas and carbon source respectively, for preparation of MWCNTs using CVD methods at 800 °C. MWCNTs were allowed to grow for 30 min on the catalyst spread on an alumina boat in a quartz tube. The materials were subsequently characterized through X-ray diffraction, Fourier transform infrared spectroscopy, surface area analysis, field emission scanning electron microscopy and transmission electron microscopy. It was determined that size and yield of MWCNTs varied depending on the type of LDH catalyst precursor that is used during synthesis. MWCNTs obtained using CoNiAl-LDH as the catalyst precursor showed smaller diameter and higher yield compared to FeCoNiAl and FeNiAl LDHs.

  12. Hydrogenation of Anthracene in Supercritical Carbon Dioxide Solvent Using Ni Supported on Hβ-Zeolite Catalyst

    Directory of Open Access Journals (Sweden)

    Ashraf Aly Hassan

    2012-01-01

    Full Text Available Catalytic hydrogenation of anthracene was studied over Ni supported on Hβ-zeolite catalyst under supercritical carbon dioxide (sc-CO2 solvent. Hydrogenation of anthracene in sc-CO2 yielded 100% conversion at 100 °C, which is attributed to the reduced mass transfer limitations, and increased solubility of H2 and substrate in the reaction medium. The total pressure of 7 MPa was found to be optimum for high selectivity of octahydroanthracene (OHA. The conversion and selectivity for OHA increased with an increase in H2 partial pressure, which is attributed to higher concentration of hydrogen atoms at higher H2 pressures. The selectivity reduced the pressure below 7 MPa because of enhanced desorption of the tetrahydro-molecules and intermediates from Ni active sites, due to higher solubility of the surface species in sc-CO2. The selectivity of OHA increased with the increase in catalyst weight and reaction time. The rate of hydrogenation of anthracene was compared with that found for napthalene and phenanthrene. The use of acetonitrile as co-solvent or expanded liquid with CO2 decreased the catalytic activity.

  13. The Effect of K and Acidity of NiW-Loaded HY Zeolite Catalyst for Selective Ring Opening of 1-Methylnaphthalene.

    Science.gov (United States)

    Lee, You-Jin; Kim, Eun-Sang; Kim, Jeong-Rang; Kim, Joo-Wan; Kim, Tae-Wan; Chae, Ho-Jeong; Kim, Chul-Ung; Lee, Chang-Ha; Jeong, Soon-Yong

    2016-05-01

    Bi-functional catalysts were prepared using HY zeolites with various SiO2/Al2O3 ratios for acidic function, NiW for metallic function, and K for acidity control. 1-Methylnaphthalene was selected as a model compound for multi-ring aromatics in heavy oil, and its selective ring opening reaction was investigated using the prepared bi-functional catalysts with different levels of acidity in a fixed bed reactor system. In NiW/HY catalysts without K addition, the acidity decreased with the SiO2/Al2O3 mole ratio of the HY zeolite. Ni1.1W1.1/HY(12) catalyst showed the highest acidity but slightly lower yields for the selective ring opening than Ni1.1W1.1/HY(30) catalyst. The acidity of the catalyst seemed to play an important role as the active site for the selective ring opening of 1-methylnaphthalene but there should be some optimum catalyst acidity for the reaction. Catalyst acidity could be controlled between Ni1.1W1.1/HY(12) and Ni1.1W1.1/HY(30) by adding a moderate amount of K to Ni1.1W1.1/HY(12) catalyst. K0.3Ni1.1W1.1/HY(12) catalyst should have the optimum acidity for the selective ring opening. The addition of a moderate amount of K to the NiW/HY catalyst must improve the catalytic performance due to the optimization of catalyst acidity.

  14. 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.

  15. Hexagonal boron nitride supported mesoSiO2-confined Ni catalysts for dry reforming of methane.

    Science.gov (United States)

    Cao, Yang; Lu, Meirong; Fang, Jianhui; Shi, Liyi; Zhang, Dengsong

    2017-07-04

    Based on the superior chemical and thermal stability of hexagonal boron nitride (h-BN), we design and synthesize h-BN supported mesoSiO2-confined Ni catalysts with a stable architecture. The as-prepared catalyst exhibits excellent coke- and sintering-resistance performance in the dry reforming of methane, and especially, there is almost no loss of activity even after a 100 h stability test due to the synergistic effects of the h-BN interface and Ni nanoparticles.

  16. An in-depth understanding of the bimetallic effects and coked carbon species on an active bimetallic Ni(Co)/Al2O3 dry reforming catalyst.

    Science.gov (United States)

    Liao, Xin; Gerdts, Rihards; Parker, Stewart F; Chi, Lina; Zhao, Yongxiang; Hill, Martyn; Guo, Junqiu; Jones, Martin O; Jiang, Zheng

    2016-06-29

    Ni/Al2O3, Co/Al2O3 and bimetallic Ni(Co)/Al2O3 catalysts were prepared using an impregnation method and employed in CO2 dry reforming of methane under coking-favored conditions. The spent catalysts were carefully characterized using typical characterization technologies and inelastic neutron scattering spectroscopy. The bimetallic catalyst exhibited a superior activity and anti-coking performance compared to Ni/Al2O3, while the most resistant to coking behavior was Co/Al2O3. The enhanced activity of the Ni(Co)/Al2O3 bimetallic catalyst is attributed to the reduced particle size of metallic species and resistance to forming stable filamentous carbon. The overall carbon deposition on the spent bimetallic catalyst is comparable to that of the spent Ni/Al2O3 catalyst, whereas the carbon deposited on the bimetallic catalyst is mainly less-stable carbonaceous species as confirmed by SEM, TPO, Raman and INS characterization. This study provides an in depth understanding of alloy effects in catalysts, the chemical nature of coked carbon on spent Ni-based catalysts and, hopefully, inspires the creative design of a new bimetallic catalyst for dry reforming reactions.

  17. Ni/Ce-MCM-41 mesostructured catalysts for simultaneous production of hydrogen and nanocarbon via methane decomposition

    Energy Technology Data Exchange (ETDEWEB)

    Guevara, J.C.; Wang, J.A.; Chen, L.F.; Valenzuela, M.A. [ESIQIE, Instituto Politecnico Nacional, Col. Zacatenco, Av. Politecnico s/n, 07738 Mexico D. F. (Mexico); Salas, P. [Centro de Fisica Aplicada y Tecnologia Avanzada, Universidad Nacional Autonoma de Mexico, Apartado Postal 1-1010, Queretaro 76000 (Mexico); Garcia-Ruiz, A. [UPIICSA, Instituto Politecnico Nacional, Te 950 Col. Granjas-Mexico, 08400 Mexico D.F. (Mexico); Toledo, J.A.; Cortes-Jacome, M.A.; Angeles-Chavez, C. [Programa de Molecular Ingenieria, Instituto Mexicano del Petroleo, Eje Lazaro Cardenas 152, 07730 Mexico D. F. (Mexico); Novaro, O. [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, A. P. 20-364, 01000 Mexico D.F. (Mexico)

    2010-04-15

    For the first time, simultaneous production of hydrogen and nanocarbon via catalytic decomposition of methane over Ni-loaded mesoporous Ce-MCM-41 catalysts was investigated. The catalytic performance of the Ni/Ce-MCM-41 catalysts is very stable and the reaction activity remained almost unchanged during 1400 min steam on time at temperatures 540, 560 and 580 C, respectively. The methane conversion level over these catalysts reached 60-75% with a 100% selectivity towards hydrogen. TEM observations revealed that most of the Ni particles located on the tip of the carbon nanofibers/nanotubes in the used catalysts, keeping their exposed surface clean during the test and thus remaining active for continuous reaction without obvious deactivation. Two kinds of carbon materials, graphitic carbon (C{sub g}) as major and amorphous carbon (C{sub A}) as minor were produced in the reaction, as confirmed by XRD analysis and TEM observations. Carbon nanofibers/nanotubes had an average diameter of approximately 30-50 nm and tens micrometers in length, depending on the reaction temperature, reaction time and Ni particle diameter. Four types of carbon nanofibers/nanotubes were detected and their formations greatly depend on the reaction temperature, time on steam and degree of the interaction between the metallic Ni and support. The respective mechanisms of the formation of nanocarbons were postulated and discussed. (author)

  18. Glucose- and Cellulose-Derived Ni/C-SO3H Catalysts for Liquid Phase Phenol Hydrodeoxygenation

    Energy Technology Data Exchange (ETDEWEB)

    Kasakov, Stanislav; Zhao, Chen; Barath, Eszter; Chase, Zizwe A.; Fulton, John L.; Camaioni, Donald M.; Vjunov, Aleksei; Shi, Hui; Lercher, Johannes A.

    2015-01-19

    Sulfonated carbons were explored as functionalized supports for Ni nanoparticles to hydrodeoxygenate (HDO) phenol. Both hexadecane and water were used as solvents. The dual-functional Ni catalysts supported on sulfonated carbon (Ni/C-SO3H) showed high rates for phenol hydrodeoxygenation in liquid hexadecane, but not in water. Glucose and cellulose were precursors to the carbon supports. Changes in the carbons resulting from sulfonation of the carbons resulted in variations of carbon sheet structures, morphologies and the surface concentrations of acid sites. While the C-SO3H supports were active for cyclohexanol dehydration in hexadecane and water, Ni/C-SO3H only catalyzed the reduction of phenol to cyclohexanol in water. The state of 3 – 5 nm grafted Ni particles was analyzed by in situ X-ray absorption spectroscopy. The results show that the metallic Ni was rapidly formed in situ without detectable leaching to the aqueous phase, suggesting that just the acid functions on Ni/C-SO3H are inhibited in presence of water. Using in situ IR spectroscopy, it was shown that even in hexadecane, phenol HDO is limited by the dehydration step. Thus, phenol HDO catalysis was further improved by physically admixing C-SO3H with the Ni/C-SO3H catalyst to balance the two catalytic functions. The minimum addition of 7 wt.% C-SO3H to the most active of the Ni/C-SO3H catalysts enabled nearly quantitative conversion of phenol and the highest selectivity (90%) towards cyclohexane in 6 h, at temperatures as low as 473 K, suggesting that the proximity to Ni limits the acid properties of the support.

  19. Self-forming graphene/Ni patterns on sapphire utilizing the pattern-controlled catalyst metal agglomeration technique

    Science.gov (United States)

    Miyoshi, Makoto; Arima, Yukinori; Kubo, Toshiharu; Egawa, Takashi

    2017-01-01

    We fabricated graphene/Ni patterns directly on sapphire substrates through a self-forming process utilizing the pattern-controlled catalyst metal agglomeration technique, which was accomplished via a thermal annealing process of rectangular Ni patterns preformed on thin amorphous carbon films on sapphire. It was confirmed that graphene films were synthesized along with the preformed Ni patterns as a result of the progress of Ni agglomeration. Notably, a few-layer graphene film was observed in specific areas along the periphery of the preformed Ni patterns. The self-forming graphene/Ni patterns showed ohmic conductivity with a contact resistance ranging from 4 × 104 to 7 × 104 Ω μm.

  20. An Effective Pd–Ni2P/C Anode Catalyst for Direct Formic Acid Fuel Cells

    OpenAIRE

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

    2014-01-01

    The direct formic acid fuel cell is an emerging energy conversion device for which palladium is considered as the state-of-the-art anode catalyst. In this communication, we show that the activity and stability of palladium for formic acid oxidation can be significantly enhanced using nickel phosphide (Ni2P) nanoparticles as a cocatalyst. X-ray photoelectron spectroscopy (XPS) reveals a strong electronic interaction between Ni2P and Pd. A direct formic acid fuel cell incorporating the best Pd-...

  1. Hydrogen production by methanol reforming on NiAl layered double hydroxide derived catalyst: Effect of the pretreatment of the catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Qi, Caixia [Institute of Applied Catalysis, Yantai University, Yantai 264005 (China); Department of Chemistry and Chemical Engineering, Royal Military College of (Canada); Amphlett, John C.; Peppley, Brant A. [Department of Chemistry and Chemical Engineering, Royal Military College of (Canada)

    2007-12-15

    This paper presents the results of the steam reforming of methanol on an as-prepared NiAl-layered double hydroxide catalyst pretreated in two different atmospheres and then the reaction at a high temperature of 390 {sup circle} C with feed having various steam-to-methanol ratios. The product composition was found to vary significantly with the pretreatment atmosphere. High activity and stability with high selectivity for CO{sub 2} and H{sub 2} and low level CO and no methane formation in a broad range of the H{sub 2}O/CH{sub 3}OH ratio was observed when the catalyst was preheated in the diluted H{sub 2} stream. Whereas in the case of pretreatment in the reactive stream of the mixture of steam and methanol, the formation of methane and its increase with more steam in feed was obtained and with time on line the catalyst deactivated with an increase in CO formation and decreases in CO{sub 2}, H{sub 2} and CH{sub 4} production. A catalyst with optimal ratio of ionic Ni in different chemical environment is suggested to obtain an active, selective and stable reforming catalyst. (author)

  2. MAu2GeS4-Chalcogel (M = Co, Ni): Heterogeneous Intra- and Intermolecular Hydroamination Catalysts

    KAUST Repository

    Davaasuren, Bambar

    2017-08-08

    High surface area macroporous chalcogenide aerogels (chalcogels) MAu2GeS4 (M = Co, Ni) were prepared from K2Au2GeS4 precursor and Co(OAc)2 or NiCl2 by one-pot sol-gel metathesis reactions in aqueous media. The MAu2GeS4-chalcogels were screened for catalytic intramolecular hydroamination of 4-pentyn-1-amine substrate at different temperatures. 87% and 58% conversion was achieved at 100 °C, using CoAu2GeS4- and NiAu2GeS4-chalcogels respectively, and the reaction kinetics follows the first order. It was established that the catalytic performance of the aerogels is associated with the M(2+) centers present in the structure. Intermolecular hydroamination of aniline with 1-R-4-ethynylbenzene (R = -H, -OCH3, -Br, -F) was carried out at 100 °C using CoAu2GeS4-chalcogel catalyst, due to its promising catalytic performance. The CoAu2GeS4-chalcogel regioselectively converted the pair of substrates to respective Markovnikov products, (E)-1-(4-R-phenyl)-N-phenylethan-1-imine, with 38% to 60% conversion.

  3. Photocatalytic hydrogen production using polymeric carbon nitride with a hydrogenase and a bioinspired synthetic Ni catalyst.

    Science.gov (United States)

    Caputo, Christine A; Gross, Manuela A; Lau, Vincent W; Cavazza, Christine; Lotsch, Bettina V; Reisner, Erwin

    2014-10-20

    Solar-light-driven H2 production in water with a [NiFeSe]-hydrogenase (H2ase) and a bioinspired synthetic nickel catalyst (NiP) in combination with a heptazine carbon nitride polymer, melon (CN(x)), is reported. The semibiological and purely synthetic systems show catalytic activity during solar light irradiation with turnover numbers (TONs) of more than 50,000 mol H2(mol H2ase)(-1) and approximately 155 mol H2 (mol NiP)(-1) in redox-mediator-free aqueous solution at pH 6 and 4.5, respectively. Both systems maintained a reduced photoactivity under UV-free solar light irradiation (λ>420 nm). © 2014 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.

  4. Thermo-Catalytic Methane Decomposition for Hydrogen Production: Effect of Palladium Promoter on Ni-based Catalysts

    Directory of Open Access Journals (Sweden)

    Irene Lock Sow Mei

    2016-08-01

    Full Text Available Hydrogen production from the direct thermo-catalytic decomposition of methane is a promising alternative for clean fuel production. However, thermal decomposition of methane can hardly be of any practical and empirical interest in the industry unless highly efficient and effective catalysts, in terms of both catalytic activity and operational lifetime have been developed. In this study, the effect of palladium (Pd as a promoter onto Ni supported on alumina catalyst has been investigated by using co-precipitation technique. The introduction of Pd promotes better catalytic activity, operational lifetime and thermal stability of the catalyst. As expected, highest methane conversion was achieved at reaction temperature of 800 °C while the bimetallic catalyst (1 wt.% Ni -1wt.% Pd/Al2O3 gave the highest methane conversion of 70% over 15 min of time-on-stream (TOS. Interestingly, the introduction of Pd as promoter onto Ni-based catalyst also has a positive effect on the operational lifetime and thermal stability of the catalyst as the methane conversion has improved significantly over 240 min of TOS. Copyright © 2016 BCREC GROUP. All rights reserved Received: 21st January 2016; Revised: 6th February 2016; Accepted: 6th March 2016 How to Cite: Mei, I.L.S., Lock, S.S.M., Vo, D.V.N., Abdullah, B. (2016. Thermo-Catalytic Methane Decomposition for Hydrogen Production: Effect of Palladium Promoter on Ni-based Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 11 (2: 191-199 (doi:10.9767/bcrec.11.2.550.191-199 Permalink/DOI: http://dx.doi.org/10.9767/bcrec.11.2.550.191-199

  5. Highly dispersed NiW/{gamma}-Al{sub 2}O{sub 3} catalyst prepared by hydrothermal deposition method

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Hao [State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249 (China); Fan, Yu.; Bao, Xiaojun [State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249 (China); The Key Laboratory of Catalysis, China National Petroleum Corp., China University of Petroleum, Beijing 102249 (China); Shi, Gang; Liu, Haiyan [The Key Laboratory of Catalysis, China National Petroleum Corp., China University of Petroleum, Beijing 102249 (China); Liu, Zhihong [Science and Technology Management Department, PetroChina Company Ltd., World Tower, 16 Andelu, Dongcheng District, Beijing 100011 (China)

    2007-07-30

    This article describes a novel hydrothermal deposition method for preparing highly dispersed NiW/{gamma}-Al{sub 2}O{sub 3} catalysts and demonstrates its advantages over the conventional impregnation method. Via the hydrothermal precipitation reactions between sodium tungstate and hydrochloric acid and between nickel nitrate and urea, respectively, the active species W and Ni were deposited on {gamma}-Al{sub 2}O{sub 3}. In the hydrothermal deposition of WO{sub 3}, a surfactant hexadecyltrimethyl ammonium bromide (CTAB) was used to prevent the aggregation of WO{sub 3}. The characterization results obtained by means of X-ray photoelectron spectroscopy (XPS), N{sub 2} adsorption and high-resolution transmission electron microscopy (HRTEM) measurements showed that compared with the catalyst prepared by the conventional impregnation method, the catalyst with the same metal contents prepared by the hydrothermal deposition had much higher W and Ni dispersion, higher specific surface area, larger pore volume, the significantly decreased slab length and slightly increased stacking degree of sulfided W species, leading to the significantly enhanced dibenzothiophene (DBT) hydrodesulfurization (HDS) activity. The DBT HDS assessment results also revealed that the catalyst containing 17.7 wt% WO{sub 3} and 2.4 wt% NiO prepared by the hydrothermal deposition method had the similar DBT HDS activity as a commercial NiW/{gamma}-Al{sub 2}O{sub 3} catalyst containing 23 wt% WO{sub 3} and 2.6 wt% NiO, resulting in the greatly decreased amount of active metals for achieving the same HDS activity. (author)

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

    Science.gov (United States)

    Zignani, Sabrina C; Baglio, Vincenzo; Sebastián, David; Saccà, Ada; Gatto, Irene; Aricò, Antonino S

    2017-03-21

    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.

  7. OXIDATIVE-REFORMING OF METHANE AND PARTIAL OXIDATION OF METHANE REACTIONS OVER NiO/PrO2/ZrO2 CATALYSTS: EFFECT OF NICKEL CONTENT

    Directory of Open Access Journals (Sweden)

    Y. J. O. Asencios

    Full Text Available Abstract In this work the behavior of NiO-PrO2-ZrO2 catalysts containing various nickel loadings was evaluated in the partial oxidation of methane and oxidative-reforming reactions of methane. The catalysts were characterized by X-Ray Diffraction Analysis (in situ-XRD, Temperature Programmed Reduction (H2-TPR, Scanning Electron Microscopy (SEM/EDX and Adsorption-Desorption of nitrogen (BET area. The reactions were carried out at 750 °C and 1 atm for 5 hours. The catalysts were studied with different nickel content: 0, 5, 10 and 15% (related to total weight of catalyst, wt%. In both reactions, the catalyst containing the mixture of the three oxides (NiO/PrO2/ZrO2 with 15% nickel (15NiPrZr catalyst showed the best activity for the conversion of the reactants into Syngas and showed high selectivity for H2 and CO. The results suggest that the promoter PrO2 and the Niº centers are in a good proportion in the catalyst with 15% Ni. Our results showed that low nickel concentrations in the catalyst led to high metallic dispersion; however, very low nickel concentrations did not favor the methane transformation into Syngas. The catalyst containing only NiO/ZrO2 in the mixture was not sufficient for the catalysis. The presence of the promoter PrO2 was very important for the catalysis of the POM.

  8. Hydroprocessing of Jatropha Oil for Production of Green Diesel over Non-sulfided Ni-PTA/Al2O3 Catalyst

    Science.gov (United States)

    Liu, Jing; Lei, Jiandu; He, Jing; Deng, Lihong; Wang, Luying; Fan, Kai; Rong, Long

    2015-01-01

    The non-sulfided Ni-PTA/Al2O3 catalyst was developed to produce green diesel from the hydroprocessing of Jatropha oil. The Ni-PTA/Al2O3 catalyst was prepared by one-pot synthesis of Ni/Al2O3 with the co-precipitation method and then impregnanting Ni/Al2O3 with PTA solution. The catalysts were characterized with BET, SEM-EDX, TEM, XRD, XPS, TGA and NH3-TPD. The Ni and W species of the Ni-PTA/Al2O3 catalyst were much more homogeneously distributed on the surface than that of commercial Al2O3. Catalytic performance in the hydroprocessing of Jatropha oil was evaluated by GC. The maximum conversion of Jatropha oil (98.5 wt%) and selectivity of the C15-C18 alkanes fraction (84.5 wt %) occurred at 360 °C, 3.0 MPa, 0.8 h−1. The non-sulfided Ni-PTA/Al2O3 catalyst is more environmentally friendly than the conventional sulfided hydroprocessing catalyst, and it exhibited the highest catalytic activity than the Ni-PTA catalyst supported with commercial Al2O3 grain and Al2O3 powder. PMID:26162092

  9. Kinetics for Steam and CO2 Reforming of Methane Over Ni/La/Al2O3 Catalyst.

    Science.gov (United States)

    Park, Myung Hee; Choi, Bong Kwan; Park, Yoon Hwa; Moon, Dong Ju; Park, Nam Cook; Kim, Young Chul

    2015-07-01

    Kinetic studies of mixed (steam and dry) reforming of methane on Ni/La/Al2O3 and Ni/La-Co (1, 3 wt%)/Al2O3 catalysts were performed in an atmospheric fixed-bed reactor. Kinetic parameters for the mixed reforming over these catalysts were obtained under reaction conditions free from heat and mass transfer limitations. Variables for the mixed reforming were the reaction temperature and partial pressure of reactants. The fitting of the experimental data for the rate of methane conversion, rCH4, using the power law rate equation rCH4 = k(PrCH4)α(PCO2)β(PH2O)γ showed that the reaction orders α, β, and γ are steady and obtained values equal to α = 1, β = 0, and γ = 0. In other words, among CH4, CO2, H2O, and H2, only CH4 reaction orders were not zero and they were affected by the promoters. The apparent activation energy on catalysts Ni/La/Al2O3, Ni/La-Co (1)/Al2O3 and Ni/La-Co (3)/Al2O3 is 85.2, 93.8, and 99.4 kJ/mol, respectively. The addition of Co to Ni/La/Al2O3 was increased the apparent activation energy of the mixed reforming reaction. And the Ni/La-Co (3 wt%)/Al2O3 catalyst showed the highest reforming activity and apparent activation energy. The Co promoters can increase the apparent activation energy of mixed reforming of methane.

  10. In situ reactivation of passivated Ni-on-alumina catalysts for toluene hydrogenation in a dielectric field

    NARCIS (Netherlands)

    Vos, B.; Poels, E.; Bliek, A.

    2002-01-01

    In recent years quite some research has been carried out in microwave-assisted catalysis and in microwave-assisted catalyst synthesis. Presently we have tested the use of dielectric fields for in situ reactivation of passivated Ni-on-alumina using dielectric fields. As a model catalytic reaction,

  11. Preparation and characterization of Ni based on natural zeolite catalyst for citronellol conversion to 3,7-Dimethyl-1-Octanol

    Science.gov (United States)

    Sudiyarmanto, Hidayati, Luthfiana N.; Kristiani, Anis; Ghaisani, Almira; Sukandar, Dede; Adilina, Indri B.; Tursiloadi, Silvester

    2017-11-01

    Citronella oil is a kind of essential oil that contains three main components, namely citronellal, citronellol, and geraniol. The high demand of citronellal and geraniol derivative prompted scientists to develop methods which are stereo-selective synthesis. A hydrogenation reaction using heterogeneous catalyst is one way of synthesis of citronella oil derivatives. In this research, synthesis of citronellol oil derivatives using Ni based on natural zeolite (Ni/ZAB) catalyst which is expected to produce the compound of 3,7-dimethyl-1-octanol. The catalyst was prepared by supporting Ni on natural zeolite by impregnation method. The physical and chemical properties of Ni/ZAB catalyst have been characterized by TGA, BET, XRD and FTIR instrumentations. Variation of pressure and temperature reactions were conducted to determine the optimum conditions for the hydrogenation of citronellol. The products from this reaction were analyzed using GC-MS instrumentation. The yield and selectivity of 3,7-dimethyl-1-octanol compound were achieved with optimum conditions at 200°C and 20 bar during 3 hours which produced around 51.97% and 47.81% respectively.

  12. Solvent free depolymerization of Kraft lignin to alkyl-phenolics using supported NiMo and CoMo catalysts

    NARCIS (Netherlands)

    Kumar, Chowdari Ramesh; Anand, Narani; Kloekhorst, Arjan; Cannilla, Catia; Bonura, Giuseppe; Frusteri, Francesco; Barta, Katalin; Heeres, Hero Jan

    2015-01-01

    The catalytic hydrotreatment of Kraft lignin using sulfided NiMo and CoMo catalysts on different acidic and basic supports (Al2O3, ZSM-5, activated carbon (AC) and MgO-La2O3) was studied in the absence of a solvent. Experiments were carried out in a batch set-up at a reaction temperature of 350

  13. Water-Gas Shift and CO Methanation Reactions over Ni-CeO2(111) Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    S Senanayake; J Evans; S Agnoli; L Barrio; T Chen; J Hrbek; J Rodriguez

    2011-12-31

    X-ray and ultraviolet photoelectron spectroscopies were used to study the interaction of Ni atoms with CeO{sub 2}(111) surfaces. Upon adsorption on CeO{sub 2}(111) at 300 K, nickel remains in a metallic state. Heating to elevated temperatures (500-800 K) leads to partial reduction of the ceria substrate with the formation of Ni{sup 2+} species that exists as NiO and/or Ce{sub 1-x}Ni{sub x}O{sub 2-y}. Interactions of nickel with the oxide substrate significantly reduce the density of occupied Ni 3d states near the Fermi level. The results of core-level photoemission and near-edge X-ray absorption fine structure point to weakly bound CO species on CeO{sub 2}(111) which are clearly distinguishable from the formation of chemisorbed carbonates. In the presence of Ni, a stronger interaction is observed with chemisorption of CO on the admetal. When the Ni is in contact with Ce{sup +3} cations, CO dissociates on the surface at 300 K forming NiC{sub x} compounds that may be involved in the formation of CH{sub 4} at higher temperatures. At medium and large Ni coverages (>0.3 ML), the Ni/CeO{sub 2}(111) surfaces are able to catalyze the production of methane from CO and H{sub 2}, with an activity slightly higher than that of Ni(100) or Ni(111). On the other hand, at small coverages of Ni (<0.3 ML), the Ni/CeO{sub 2}(111) surfaces exhibit a very low activity for CO methanation but are very good catalysts for the water-gas shift reaction.

  14. Carbon Dioxide Dry Reforming of Glycerol for Hydrogen Production using Ni/ZrO2 and Ni/CaO as Catalysts

    Directory of Open Access Journals (Sweden)

    Nur Nabillah Mohd Arif

    2016-08-01

    Full Text Available Glycerol, byproduct from the biodiesel production can be effectively utilized as the promising source of synthesis gas (syngas through a dry reforming reaction. Combination of these waste materials with greenhouse gases which is carbon dioxide (CO2 will help to reduce environmental problem such as global warming. This dry reforming reaction has been carried out in a fixed bed batch reactor at 700 °C under the atmospheric pressure for 3 hours. In this experiment, reforming reaction was carried out using Nickel (Ni as based catalyst and supported with zirconium (ZrO2 and calcium (CaO oxides. The catalysts were prepared by wet impregnation method and characterized using Bruanaer-Emmett-Teller (BET surface area, Scanning Electron Microscopy (SEM, X-ray Diffraction (XRD, Thermo Gravimetric (TGA, and Temperature Programmed Reduction (TPR analysis. Reaction studies show that 15% Ni/CaO give the highest hydrogen yield and glycerol conversion that peaked at 24.59% and 30.32%, respectively. This result is verified by XRD analysis where this catalyst shows low crystallinity and fine dispersion of Ni species resulted in high specific surface area which gives 44.93 m2/g that is validated by BET.  Copyright © 2016 BCREC GROUP. All rights reserved Received: 21st January 2016; Revised: 24th February 2016; Accepted: 29th February 2016 How to Cite: Arif, N.M.M., Vo, D.V.N., Azizan,M.T., Abidin S.Z. (2016. Carbon Dioxide Dry Reforming of Glycerol for Hydrogen Production using Ni/ZrO2 and Ni/CaO as Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 11 (2: 200-209 (doi:10.9767/bcrec.11.2.551.200-209 Permalink/DOI: http://dx.doi.org/10.9767/bcrec.11.2.551.200-209

  15. Processing of spent NiW/Al{sub 2}O{sub 3} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Paulino, Jessica Frontino; Afonso, Julio Carlos, E-mail: julio@iq.ufrj.br [Departamento de Quimica Analitica, Instituto de Quimica, Universidade Federal do Rio de Janeiro, RJ (Brazil); Cunha, Jose Waldemar Silva Dias da [Instituto de Engenharia Nuclear (IEN/CNEN-RJ), RJ (Brazil). Departamento de Quimica e Materiais Nucleares

    2013-09-01

    Spent oxidized (500 deg C, 5 h) commercial NiW/Al{sub 2}O{sub 3} catalysts were processed using two different routes: a) fusion with NaOH (650 deg C, 1 h), the roasted mass was leached in water; b) leaching with HCl or H{sub 2}SO{sub 4} (70 deg C, 1-3 h). HCl was the best leachant. In both routes, soluble tungsten was extracted at pH 1 with Alamine 336 (10 vol.% in kerosene) and stripped with 2 mol L{sup -1} NH{sub 4}OH (25 deg C, one stage, aqueous/organic ratio = 1 v/v). Tungsten was isolated as ammonium paratungstate at very high yield (> 97.5%). The elements were better separated using the acidic route. (author)

  16. Processing of spent NiW/Al2O3 catalysts

    Directory of Open Access Journals (Sweden)

    Jéssica Frontino Paulino

    2013-01-01

    Full Text Available Spent oxidized (500 ºC, 5 h commercial NiW/Al2O3 catalysts were processed using two different routes: a fusion with NaOH (650 ºC, 1 h, the roasted mass was leached in water; b leaching with HCl or H2SO4 (70 ºC, 1-3 h. HCl was the best leachant. In both routes, soluble tungsten was extracted at pH 1 with Alamine 336 (10 vol.% in kerosene and stripped with 2 mol L-1 NH4OH (25 ºC, one stage, aqueous/organic ratio = 1 v/v. Tungsten was isolated as ammonium paratungstate at very high yield (> 97.5%. The elements were better separated using the acidic route.

  17. Hydrogen production from glycerol on Ni/Al{sub 2}O{sub 3} catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Sanchez, Esteban A.; D' Angelo, Miguel A.; Comelli, Raul A. [Instituto de Investigaciones en Catalisis y Petroquimica - INCAPE (F.I.Q.-U.N.L., CONICET), Santiago del Estero 2654, S3000AOJ - Santa Fe (Argentina)

    2010-06-15

    The growing demand of hydrogen needs renewable sources of raw materials to produce it. Glycerol, by-product of biodiesel synthesis, could be a bio-renewable substrate to obtain hydrogen. A Ni(5.8%)-alumina catalyst was evaluated in the steam reforming of glycerol at 600-700 C, atmospheric pressure, 16:1 water:glycerol molar ratio, and 3.4-10.0 h{sup -1} WHSV. A glycerol aqueous solution was fed, while a nitrogen stream was co-fed. After 4 h-on-stream, conversion was 96.8% at 600 C increasing to 99.4% at 700 C, reaching the largest hydrogen selectivity (99.7%) at 650 C. After 8 h, conversion decreases more significantly at 600 C, while the hydrogen selectivity does not significantly change with temperature and increases by decreasing WHSV. After 4 h, the main by-product was methane (76-97%), increasing at higher temperature, followed by ethene, ethane, propene, and propane. At 700 C and 10.0 h{sup -1} WHSV, the main by-products were ethene (47%) and methane (37%); it could be associated to catalyst deactivation. (author)

  18. Water–Gas Shift Reaction over Ni/CeO2 Catalysts

    Directory of Open Access Journals (Sweden)

    Ludmilla Bobrova

    2017-10-01

    Full Text Available This paper reports the results of a study of a water–gas shift reaction over nickel–ceria catalysts with different metal loading. Within this study, the overall CO conversion and observed kinetic behavior were investigated over the temperature range of 250–550 °C in different reactor configurations (fixed-bed and microchannel reactors. The quasi-steady state kinetics of the CO water–gas shift reaction was studied for fractions of Ni-containing cerium oxide catalysts in fixed-bed experiments at lab-scale level using a very dilute gas (1% CO + 1.8% H2O in Не. A set of experiments with a microchannel reactor was performed using the feed composition (CO:H2O:H2:N2 = 1:2:2:2, representing a product gas from methane partial oxidation. The results were interpreted using computational models. The kinetic parameters were determined by regression analysis, while mechanistic aspects were considered only briefly. Simulation of the WGS reaction in the microreactor was also carried out by using the COMSOL Multiphysics program.

  19. In situ study of atomic structure transformations of Pt-Ni nanoparticle catalysts during electrochemical potential cycling.

    Science.gov (United States)

    Tuaev, Xenia; Rudi, Stefan; Petkov, Valeri; Hoell, Armin; Strasser, Peter

    2013-07-23

    When exposed to corrosive anodic electrochemical environments, Pt alloy nanoparticles (NPs) undergo selective dissolution of the less noble component, resulting in catalytically active bimetallic Pt-rich core-shell structures. Structural evolution of PtNi6 and PtNi3 NP catalysts during their electrochemical activation and catalysis was studied by in situ anomalous small-angle X-ray scattering to obtain insight in element-specific particle size evolution and time-resolved insight in the intraparticle structure evolution. Ex situ high-energy X-ray diffraction coupled with pair distribution function analysis was employed to obtain detailed information on the atomic-scale ordering, particle phases, structural coherence lengths, and particle segregation. Our studies reveal a spontaneous electrochemically induced formation of PtNi particles of ordered Au3Cu-type alloy structures from disordered alloy phases (solid solutions) concomitant with surface Ni dissolution, which is coupled to spontaneous residual Ni metal segregation during the activation of PtNi6. Pt-enriched core-shell structures were not formed using the studied Ni-rich nanoparticle precursors. In contrast, disordered PtNi3 alloy nanoparticles lose Ni more rapidly, forming Pt-enriched core-shell structures with superior catalytic activity. Our X-ray scattering results are confirmed by STEM/EELS results on similar nanoparticles.

  20. 3D-nanoarchitectured Pd/Ni catalysts prepared by atomic layer deposition for the electrooxidation of formic acid

    Directory of Open Access Journals (Sweden)

    Loïc Assaud

    2014-02-01

    Full Text Available Three-dimensionally (3D nanoarchitectured palladium/nickel (Pd/Ni catalysts, which were prepared by atomic layer deposition (ALD on high-aspect-ratio nanoporous alumina templates are investigated with regard to the electrooxidation of formic acid in an acidic medium (0.5 M H2SO4. Both deposition processes, Ni and Pd, with various mass content ratios have been continuously monitored by using a quartz crystal microbalance. The morphology of the Pd/Ni systems has been studied by electron microscopy and shows a homogeneous deposition of granularly structured Pd onto the Ni substrate. X-ray diffraction analysis performed on Ni and NiO substrates revealed an amorphous structure, while the Pd coating crystallized into a fcc lattice with a preferential orientation along the [220]-direction. Surface chemistry analysis by X-ray photoelectron spectroscopy showed both metallic and oxide contributions for the Ni and Pd deposits. Cyclic voltammetry of the Pd/Ni nanocatalysts revealed that the electrooxidation of HCOOH proceeds through the direct dehydrogenation mechanism with the formation of active intermediates. High catalytic activities are measured for low masses of Pd coatings that were generated by a low number of ALD cycles, probably because of the cluster size effect, electronic interactions between Pd and Ni, or diffusion effects.

  1. Role of CeO2 promoter in NiO/α-Al2O3 catalyst for dry reforming of methane

    Science.gov (United States)

    Loc, Luu Cam; Phuong, Phan Hong; Tri, Nguyen

    2017-09-01

    A series of Ni/α-Al2O3 (NiAl) catalysts promoted by CeO2 was prepared by co-impregnation methods with content of (NiO+CeO2) being in the range of 10-30 wt%. The NiO:CeO2 weight ratio was fluctuated at 1:1, 1:2 and 1:3. Several techniques, including X-ray powder diffraction (XRD), Hydrogen temperature-programmed reduction (H2-TPR), and transmission electron microscopy (TEM) were used to investigate catalysts' physico-chemical properties. The activity of these catalysts in dry reforming of CH4 was investigated at temperature range of 550-800 °C. The results revealed that the most suitable CeO2 promoted Ni catalyst contained 20 wt% of (NiO+CeO2) and NiO:CeO2 weight ratio of 1:2. The best catalytic performance of catalyst [20(1Ni2Ce)Al] due to a better reducibility resulted in a higher amount of free small particle NiO. At 700 °C and CH4:CO2 molar ratio of 1:1, the conversion of CH4 and CO2 on the most suitable CeO2 promoted Ni catalyst reached 86% and 67%, respectively; H2 and CO selectivity of 90% and H2:CO molar ratio of 1.15 were obtained. Being similar to MgO [1], promoter CeO2 could improve catalytic activity of Ni/α-Al2O3 catalyst at a lower range of temperature. Besides, both MgO and CeO2 had a great impact on improving coke resistance of Ni catalysts. At higher temperature, the role of CeO2 as well as MgO in preventing coke formation on catalyst was clarified by temperature-programmed oxidation (TPO) technique. Coke amount formed after 30-h TOS on 20(1Ni2Ce) catalyst was found to be 22.18 mgC/gcat, being less than on non-promoted catalyst (36.75 mgC/gcat), but more than on 20(1Ni2Mg)Al one (5.25 mgC/gcat).

  2. Kinetics of germanium nanowire growth by the vapor-solid-solid mechanism with a Ni-based catalyst

    Directory of Open Access Journals (Sweden)

    Shruti V. Thombare

    2013-12-01

    Full Text Available The kinetics of vapor-solid-solid (VSS Ge nanowire growth using a Ni-based catalyst were investigated to probe the rate-limiting step for this complex nanoscale crystal growth process. The effects of key parameters such as temperature and precursor partial pressure on the nanowire growth rate were studied in order to gain detailed insights into the growth kinetics. Two different regimes were observed for VSS growth of Ge nanowires as function of temperature. At higher temperatures (345 °C–375 °C, kinetics data suggest that mass transport of germane precursor to the catalyst surface is rate limiting. At lower temperatures (<345 °C, either surface reaction of the GeH4 precursor on the catalyst or incorporation of Ge into the nanowire across the wire/catalyst interface is rate limiting.

  3. Phase Composition of Ni/Mg1−xNixO as a Catalyst Prepared for Selective Methanation of CO in H2-Rich Gas

    Directory of Open Access Journals (Sweden)

    Mengmeng Zhang

    2015-01-01

    Full Text Available Supported Ni catalysts Ni/Mg1−xNixO were prepared by reducing samples NiO-MgO in H2/N2 mixture gas at 500°C~800°C for selective methanation of CO in H2-rich gas (CO-SMET. The samples NiO-MgO were obtained by heating water slurry of MgO and Ni(NO32 in a rotary evaporator at 80°C and a final calcination in air at 400°C~800°C. X-ray diffraction (XRD and temperature programmed reduction (TPR measurements demonstrate that the samples NiO-MgO were composed of solid solution Mg1−yNiyO as the main phase and a minor amount of NiO at calcination temperature of 400°C, and amount of the NiO was decreased as calcination temperature increased. Phase composition of the catalysts Ni/Mg1−xNixO was estimated by the Rietveld method. Effects of reduction temperature, feed Ni/Mg ratio, and calcination temperature on phase composition and catalytic activity of the catalysts were investigated. It is clear that CO conversion was generally enhanced by an increased amount of metallic Ni of the catalysts.

  4. Novel Anion Exchange Resin-based Catalyst for Liquid-phase Methanol Synthesis at 373–393 K

    National Research Council Canada - National Science Library

    Aika, Ken-ichi; Kobayashi, Hidenobu; Harada, Kenji; Inazu, Koji

    2004-01-01

    A thermo-stable anion exchange resin–Raney Cu system was found as the most effective solid catalyst for low-temperature liquid-phase methanol synthesis at 373 to 393 K under 5.0 MPa of syngas (2H2/CO). With the catalyst...

  5. Syngas Production from CO2 Reforming and CO2-steam Reforming of Methane over Ni/Ce-SBA-15 Catalyst

    Science.gov (United States)

    Tan, J. S.; Danh, H. T.; Singh, S.; Truong, Q. D.; Setiabudi, H. D.; Vo, D.-V. N.

    2017-06-01

    This study compares the catalytic performance of mesoporous 10 Ni/Ce-SBA-15 catalyst for CO2 reforming and CO2-steam reforming of methane reactions in syngas production. The catalytic performance of 10 Ni/Ce-SBA-15 catalyst for CO2 reforming and CO2-steam reforming of methane was evaluated in a temperature-controlled tubular fixed-bed reactor at stoichiometric feed composition, 1023 K and atmospheric pressure for 12 h on-stream with gas hourly space velocity (GHSV) of 36 L gcat -1 h-1. The 10 Ni/Ce-SBA-15 catalyst possessed a high specific BET surface area and average pore volume of 595.04 m2 g-1. The XRD measurement revealed the presence of NiO phase with crystallite dimension of about 13.60 nm whilst H2-TPR result indicates that NiO phase was completely reduced to metallic Ni0 phase at temperature beyond 800 K and the reduction temperature relied on different degrees of metal-support interaction associated with the location and size of NiO particles. The catalytic reactivity was significantly enhanced with increasing H2O/CO2 feed ratio. Interestingly, the H2/CO ratio for CO2-steam reforming of methane varied between 1 and 3 indicated the occurrence of parallel reactions, i.e., CH4 steam reforming giving a H2/CO of 3 whilst reverse water-gas shift (RWGS) reaction consuming H2 to produce CO gaseous product.

  6. Effects of adding lanthanum to Ni/ZrO{sub 2} catalysts on ethanol steam reforming; Efeito da adicao de lantanio em catalisadores de Ni/ZrO{sub 2} aplicados na reacao de reforma a vapor de etanol

    Energy Technology Data Exchange (ETDEWEB)

    Profeti, Luciene Paula Roberto [Centro de Ciencias Agrarias, Universidade Federal do Espirito Santo, Alegre, ES (Brazil); Habitzheuter, Filipe; Assaf, Elisabete Moreira, E-mail: eassaf@iqsc.usp.br [Instituto de Quimica de Sao Carlos, Universidade de Sao Paulo, Sao Carlos, SP (Brazil)

    2012-07-01

    The catalytic performance of Ni/ZrO{sub 2} catalysts loaded with different lanthanum content for steam reforming of ethanol was investigated. Catalysts were characterized by BET surface area, X-ray diffraction, UV-vis spectroscopy, temperature programmed reduction, and X-ray absorption fine structure techniques. Results showed that lanthanum addition led to an increase in the degree of reduction of both NiO and nickel surface species interacting with the support, due to the higher dispersion effect. The best catalytic performance at 450 deg C was found for the Ni/12LZ catalyst, which exhibited an effluent gaseous mixture with the highest H{sub 2} yield. (author)

  7. Oxidation of CO and Methanol on Pd-Ni Catalysts Supported on Different Chemically-Treated Carbon Nanofibers

    Directory of Open Access Journals (Sweden)

    Juan Carlos Calderón

    2016-10-01

    Full Text Available In this work, palladium-nickel nanoparticles supported on carbon nanofibers were synthesized, with metal contents close to 25 wt % and Pd:Ni atomic ratios near to 1:2. These catalysts were previously studied in order to determine their activity toward the oxygen reduction reaction. Before the deposition of metals, the carbon nanofibers were chemically treated in order to generate oxygen and nitrogen groups on their surface. Transmission electron microscopy analysis (TEM images revealed particle diameters between 3 and 4 nm, overcoming the sizes observed for the nanoparticles supported on carbon black (catalyst Pd-Ni CB 1:2. From the CO oxidation at different temperatures, the activation energy Eact for this reaction was determined. These values indicated a high tolerance of the catalysts toward the CO poisoning, especially in the case of the catalysts supported on the non-chemically treated carbon nanofibers. On the other hand, apparent activation energy Eap for the methanol oxidation was also determined finding—as a rate determining step—the COads diffusion to the OHads for the catalysts supported on carbon nanofibers. The results here presented showed that the surface functional groups only play a role in the obtaining of lower particle sizes, which is an important factor in the obtaining of low CO oxidation activation energies.

  8. MECHANISTIC KINETIC MODELS FOR STEAM REFORMING OF CONCENTRATED CRUDE ETHANOL ON NI/AL2O3 CATALYST

    Directory of Open Access Journals (Sweden)

    O. A. OLAFADEHAN

    2015-05-01

    Full Text Available Mechanistic kinetic models were postulated for the catalytic steam reforming of concentrated crude ethanol on a Ni-based commercial catalyst at atmosphere pressure in the temperature range of 673-863 K, and at different catalyst weight to the crude ethanol molar flow rate ratio (in the range 0.9645-9.6451 kg catalyst h/kg mole crude ethanol in a stainless steel packed bed tubular microreactor. The models were based on Langmuir-Hinshelwood-Hougen-Watson (LHHW and Eley-Rideal (ER mechanisms. The optimization routine of Nelder-Mead simplex algorithm was used to estimate the inherent kinetic parameters in the proposed models. The selection of the best kinetic model amongst the rival kinetic models was based on physicochemical, statistical and thermodynamic scrutinies. The rate determining step for the steam reforming of concentrated crude ethanol on Ni/Al2O3 catalyst was found to be surface reaction between chemisorbed CH3O and O when hydrogen and oxygen were adsorbed as monomolecular species on the catalyst surface. Excellent agreement was obtained between the experimental rate of reaction and conversion of crude ethanol, and the simulated results, with ADD% being ±0.46.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-09-01

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

  10. Direct vs. indirect pathway for nitrobenzene reduction reaction on a Ni catalyst surface: a density functional study.

    Science.gov (United States)

    Mahata, Arup; Rai, Rohit K; Choudhuri, Indrani; Singh, Sanjay K; Pathak, Biswarup

    2014-12-21

    Density functional theory (DFT) calculations are performed to understand and address the previous experimental results that showed the reduction of nitrobenzene to aniline prefers direct over indirect reaction pathways irrespective of the catalyst surface. Nitrobenzene to aniline conversion occurs via the hydroxyl amine intermediate (direct pathway) or via the azoxybenzene intermediate (indirect pathway). Through our computational study we calculated the spin polarized and dispersion corrected reaction energies and activation barriers corresponding to various reaction pathways for the reduction of nitrobenzene to aniline over a Ni catalyst surface. The adsorption behaviour of the substrate, nitrobenzene, on the catalyst surface was also considered and the energetically most preferable structural orientation was elucidated. Our study indicates that the parallel adsorption behaviour of the molecules over a catalyst surface is preferable over vertical adsorption behaviour. Based on the reaction energies and activation barrier of the various elementary steps involved in direct or indirect reaction pathways, we find that the direct reduction pathway of nitrobenzene over the Ni(111) catalyst surface is more favourable than the indirect reaction pathway.

  11. Reductive amination of ethanol to ethylamines over Ni/Al{sub 2}O{sub 3} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Park, Jun Hyun [Korea Research Institute of Chemical Technology, Daejeon (Korea, Republic of); Hong, Eunpyo; An, Sang Hee; Shin, Chae-Ho; Lim, Dong-Hee [Chungbuk National University, Chungju (Korea, Republic of)

    2017-10-15

    Ni(x)/Al{sub 2}O{sub 3} (x=wt%) catalysts with Ni loadings of 5-25 wt% were prepared via a wet impregnation method on an γ-Al{sub 2}O{sub 3} support and subsequently applied in the reductive amination of ethanol to ethylamines. Among the various catalysts prepared, Ni(10)/Al2O3 exhibited the highest metal dispersion and the smallest Ni particle size, resulting in the highest catalytic performance. To reveal the effects of reaction parameters, a reductive amination process was performed by varying the reaction temperature (T), weight hourly space velocity (WHSV), and NH{sub 3} and H{sub 2} partial pressures in the reactions. In addition, on/off experiments for NH{sub 3} and H{sub 2} were also carried out. In the absence of NH{sub 3} in the reactant stream, the ethanol conversion and selectivities towards the different ethylamine products were significantly reduced, while the selectivity to ethylene was dominant due to the dehydration of ethanol. In contrast, in the absence of H{sub 2}, the selectivity to acetonitrile significantly increased due to dehydrogenation of the imine intermediate. Although a small amount of catalyst deactivation was observed in the conversion of ethanol up to 10 h on stream due to the formation of nickel nitride, the Ni(10)/Al{sub 2}O{sub 3} catalyst exhibited stable catalytic performance over 90 h under the optimized reaction conditions (i.e., T=190 .deg. C, WHSV=0.9 h{sup -1}, and EtOH/NH{sub 3}/H{sub 2} molar ratio=1/1/6).

  12. Synthesis of MWCNTs Using Monometallic and Bimetallic Combinations of Fe, Co and Ni Catalysts Supported on Nanometric SiC via TCVD

    Directory of Open Access Journals (Sweden)

    F. Shahi

    2015-04-01

    Full Text Available Nanometric Carbid Silicon (SiC supported monometallic and bimetallic catalysts containing Fe, Co, Ni transition metals were prepared by wet impregnation method. Multiwall carbon nanotubes (MWCNTs were synthesized over the prepared catalysts from catalytic decomposition of acetylene at 850°C by thermal chemical vapor deposition (TCVD technique. The synthesized nanomaterials (catalysts and CNTs were characterized by X-ray diffraction (XRD, Scanning Electron Microscopy (SEM, Transmission Electron Microscopy (TEM and Raman spectroscopy. In this paper, using of nanometric SiC powder as catalyst support was examined and the effect of applied catalyst type on characteristics of grown CNTs was investigated. The results revealed that iron, cobalt and nickel are in oxide, cobalt ferrite (CoFe2O4 and nickel ferrite (NiFe2O4 forms and nanometric SiC powder can be applied as an appropriate catalyst support in CNT growth process. It was observed that the produced CNTs on bimetallic Fe-Co possess smaller average diameter, less amorphous carbon and denser morphology compared to other binary metallic combinations. It was found that the catalytic activity of bimetallic composition decreased in the order of Fe-Co> Fe-Ni> Co-Ni. Furthermore, the monometallic Fe catalyst has the most catalytic activity compared to monometallic Co and Ni catalysts.

  13. Production of Renewable Hydrogen from Glycerol Steam Reforming over Bimetallic Ni-(Cu,Co,Cr Catalysts Supported on SBA-15 Silica

    Directory of Open Access Journals (Sweden)

    Alicia Carrero

    2017-02-01

    Full Text Available Glycerol steam reforming (GSR is a promising alternative to obtain renewable hydrogen and help the economics of the biodiesel industry. Nickel-based catalysts are typically used in reforming reactions. However, the choice of the catalyst greatly influences the process, so the development of bimetallic catalysts is a research topic of relevant interest. In this work, the effect of adding Cu, Co, and Cr to the formulation of Ni/SBA-15 catalysts for hydrogen production by GSR has been studied, looking for an enhancement of its catalytic performance. Bimetallic Ni-M/SBA-15 (M: Co, Cu, Cr samples were prepared by incipient wetness co-impregnation to reach 15 wt % of Ni and 4 wt % of the second metal. Catalysts were characterized by inductively coupled plasma atomic emission spectroscopy (ICP-AES, N2-physisorption, X-ray powder diffraction (XRD, hydrogen temperature programmed reduction (H2-TPR, transmission electron microscopy (TEM, scanning electron microscopy (SEM, and thermogravimetric analyses (TGA, and tested in GSR at 600 °C and atmospheric pressure. The addition of Cu, Co, and Cr to the Ni/SBA-15 catalyst helped to form smaller crystallites of the Ni phase, this effect being more pronounced in the case of the Ni-Cr/SBA-15 sample. This catalyst also showed a reduction profile shifted towards higher temperatures, indicating stronger metal-support interaction. As a consequence, the Ni-Cr/SBA-15 catalyst exhibited the best performance in GSR in terms of glycerol conversion and hydrogen production. Additionally, Ni-Cr/SBA-15 achieved a drastic reduction in coke formation compared to the Ni/SBA-15 material.

  14. Synthesis of nanoporous CuO/TiO2/Pd-NiO composite catalysts by chemical dealloying and their performance for methanol and ethanol electro-oxidation

    Science.gov (United States)

    Niu, Mengying; Xu, Wence; Zhu, Shengli; Liang, Yanqin; Cui, Zhenduo; Yang, Xianjin; Inoue, Akihisa

    2017-09-01

    Nanoporous CuO/TiO2/Pd-NiO-x (x = 0, 1, 3, 5, 7 at%) catalysts have been synthesized by dealloying Cu-Ti-Pd-Ni alloy ribbons in acid solution. The nanoporous structure and chemical composition of the catalysts distribute uniformly. Based on the electrochemical active area (EASA), electrocatalytic activity and stability, the np-CuO/TiO2/Pd-NiO-3 catalyst possesses the best performance for methanol and ethanol electro-oxidation. For methanol and ethanol electro-oxidation, the anodic current densities in forward scan of the np-CuO/TiO2/Pd-NiO-3 catalyst are about 5.6 times and 2.1 times larger than that of the np-CuO/TiO2/Pd catalyst, respectively. The introduction of NiO provides more electrochemical active sites due to the improved geometrical and bifunctional mechanism. NiO promotes the adsorption of oxygen-containing species (OHads) on the catalyst surface, and electron effect between Pd and Ni is favorable for charge transfer. This accelerates the removal of intermediate products during the oxidation process. The electrocatalytic processes of methanol and ethanol oxidation in alkaline solution are controlled by both charge transfer and diffusion.

  15. Hydrogenation of the Exocyclic Olefinic Bond at C-16/C-17 Position of ent-Kaurane Diterpene Glycosides of Stevia rebaudiana Using Various Catalysts

    Science.gov (United States)

    Chaturvedula, Venkata Sai Prakash; Prakash, Indra

    2013-01-01

    Catalytic hydrogenation of the exocyclic double bond present between C16 and C17 carbons of the four ent-kaurane diterpene glycosides namely rebaudioside A, rebaudioside B, rebaudioside C, and rebaudioside D isolated from Stevia rebaudiana has been carried out using Pt/C, Pd(OH)2, Rh/C, Raney Ni, PtO2, and 5% Pd/BaCO3 to their corresponding dihydro derivatives with 17α and 17β methyl group isomers. Reactions were performed using the above-mentioned catalysts with the solvents methanol, water, and ethanol/water (8:2) under various conditions. Synthesis of reduced steviol glycosides was performed using straightforward chemistry and their structures were characterized on the basis of 1D and 2D NMR spectral data, including a comparison with reported spectral data. PMID:23896597

  16. Hydrogenation of the Exocyclic Olefinic Bond at C-16/C-17 Position of ent-Kaurane Diterpene Glycosides of Stevia rebaudiana Using Various Catalysts

    Directory of Open Access Journals (Sweden)

    Indra Prakash

    2013-07-01

    Full Text Available Catalytic hydrogenation of the exocyclic double bond present between C16 and C17 carbons of the four ent-kaurane diterpene glycosides namely rebaudioside A, rebaudioside B, rebaudioside C, and rebaudioside D isolated from Stevia rebaudiana has been carried out using Pt/C, Pd(OH2, Rh/C, Raney Ni, PtO2, and 5% Pd/BaCO3 to their corresponding dihydro derivatives with 17α and 17β methyl group isomers. Reactions were performed using the above-mentioned catalysts with the solvents methanol, water, and ethanol/water (8:2 under various conditions. Synthesis of reduced steviol glycosides was performed using straightforward chemistry and their structures were characterized on the basis of 1D and 2D NMR spectral data, including a comparison with reported spectral data.

  17. Structural and textural study of Ni and/or Co in a common molybdate lattice as catalysts

    Directory of Open Access Journals (Sweden)

    Boukhlouf H.

    2013-09-01

    Full Text Available This work deals with the search for new molybdate catalyst formulations, which are known to be active in light alkane oxidative dehydrogenation, a process which could be replace in the near future the common steam cracking and pure dehydrogenation processes currently used for the production of alkenes. Co, Ni and mixed Ni-Co molybdates of various compositions are prepared by a modified coprecipitation procedure from metal nitrates and ammonium heptamolybdate. Their structural and textural properties were studied by XRD, Raman, B.E.T and XPS. Textural and structural properties of the materials are correlated to the composition.

  18. Effect of calcination temperature on the structure and catalytic performance of 80Ni20CO/SiO2 catalyst for CO2 methanation

    Science.gov (United States)

    Md Ali, S. A.; Hamid, K. H. K.; Ismail, K. N.

    2017-09-01

    The 80Ni20Co/SiO2 catalysts prepared using co-precipitate and incipient wetness impregnation method were used for production of methane through CO2 methanation reaction between CO and H2 gases. The effect of a range of calcination temperature on the structure and catalytic performance of 80Ni20Co/SiO2 catalyst was investigated using microactivity fixed bed reactor. It was found that the catalyst calcined at 400°C for 4.5 h under air atmosphere has shown the best catalytic performance for CO2 methanation. Characterization of 80Ni20Co/SiO2 catalyst calcined fresh samples was carried out using TPR-H2 analysis, Brunauere Emmette Teller (BET) measurements and X-ray diffraction (XRD. It was observed that calcination temperature influenced the structure, morphology and catalytic performance of the catalysts.

  19. Insight into the influence of addition of a second metal Fe and supports with different morphology on H2 dissociation over Ni/MgO catalysts

    Science.gov (United States)

    Liu, Hongyan; Li, Kai; Zhang, Riguang; Ling, Lixia; Wang, Baojun

    2017-12-01

    The effect of addition of a second metal to activation component and the support with different morphology on H2 dissociation on Ni/MgO catalyst was investigated using density functional theory. The results show that after addition of a second metal Fe, the metal-support interaction is increased in perfect MgO supported Ni catalyst while it is decreased in defective MgO supported Ni catalyst. Although the change is difference between metal-support interaction, the ability of H2 dissociation is increased on the two surfaces. Analyzing those results from addition of Fe, Co and Cu to Ni/MgO, one can conclude that it is neither too strong nor too weak (i.e., medium) interaction between metal and support that favors to improve the catalyst performance.

  20. 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.

  1. Kinetic studies of CO2 methanation over a Ni/γ-Al2O3 catalyst.

    Science.gov (United States)

    Hubble, R A; Lim, J Y; Dennis, J S

    2016-10-20

    The production of methane by reacting CO2 with H2 (CO2 methanation) has the potential for producing synthetic natural gas, which could be exported using the existing infrastructure for the distribution of natural gas. The methanation of CO2 was investigated over a wide range of partial pressures of products and reactants using (i) a gradientless, spinning-basket reactor operated in batch mode and (ii) a laboratory-scale packed bed reactor operated continuously. The rate and selectivity of CO2 methanation, using a 12 wt% Ni/γ-Al2O3 catalyst, were explored at temperatures 445-497 K and pressures up to 20 bar. Research with the batch reactor showed that the rate increased with increasing partial pressures of H2 and CO2 when the partial pressures of these reactants were low; however, the rate of reaction was found to be insensitive to changes in the partial pressures of H2 and CO2 when their partial pressures were high. A convenient method of determining the effect of H2O on the rate of reaction was also developed using the batch reactor and the inhibitory effect of H2O on CO2 methanation was quantified. The kinetic measurements were compared with a mathematical model of the reactor, in which different kinetic expressions were explored. The kinetics of the reaction were found to be consistent with a mechanism in which adsorbed CO2 dissociated to adsorbed CO and O on the surface of the catalyst with the rate-limiting step being the subsequent dissociation of adsorbed CO. The ability of the kinetic expressions to predict the results from the continuous, packed-bed reactor was explored, with some discrepancies discussed.

  2. Examining the Utility of the New Raney Vocabulary Measure Alongside the WAIS-III.

    Science.gov (United States)

    Ferguson, Ryan J; Roy-Charland, Annie; Dickinson, Joël

    2018-01-29

    Psychometric tests related to vocabulary assessments are, for the most part, restricted in their use by trained professionals and/or are costly. These restrictions limit their use, especially for research purposes. To circumvent these limitations, the Raney Vocabulary Measure was created for assessing vocabulary proficiency, specifically for research purposes. The measure consists of 30 questions where participants were instructed to choose the best definition of each word. The purpose of the study was to examine the utility of the new measure using the highly standardized but protected Wechsler Adult Intelligence Scale. Results from the linear combination of the subscales revealed the significant prediction of the Raney Vocabulary Measure, with the Vocabulary subtest contributing most to the unique variance. These results support that the test examines vocabulary ability. The current results are promising as the test would allow for greater accessibility for researchers who do not have access to restricted psychometric tests.

  3. The Reduction of Nitriles to Aldehydes: Applications of Raney Nickel ...

    African Journals Online (AJOL)

    NJD

    sive in contact with oxidizers; it is not considered a fire hazard but forms spontaneously flammable phosphine gas when heated. In the absence of a metal catalyst, it has been used under microwave irradiation selectively to reduce the nitro group into an amino group; certain common functional groups including nitrile are ...

  4. Hydroconversion of methyl laurate on bifunctional Ni2P/AlMCM-41 catalyst prepared via in situ phosphorization using triphenylphosphine

    Science.gov (United States)

    Zhao, Sha; Zhang, Zhena; Zhu, Kongying; Chen, Jixiang

    2017-05-01

    A series of Ni2P/AlMCM-41-x bifunctional catalysts with different Si/Al ratios (x) were synthesized by in situ phosphorization of Ni/AlMCM-41-x with triphenylphosphine (nominal Ni/P ratio of 0.75) at 300 °C on a fixed-bed reactor. For comparison, NiP/AlMCM-41-5-TPR was also prepared by the TPR method from the supported nickel phosphate with the Ni/P ratio of 1.0, during which metallic Ni rather than Ni2P formed. TEM images show that Ni and Ni2P particles uniformly distributed in Ni2P/AlMCM-41-x and NiP/AlMCM-41-5-TPR. The Ni2P/AlMCM-41-x acidity increased with decreasing the Si/Al ratio. In the hydroconversion of methyl laurate, the conversions were close to 100% on all catalysts at 360 °C, 3.0 MPa, methyl laurate WHSV of 2 h-1 and H2/methyl laurate ratio of 25. As to Ni2P/AlMCM-41-x, with decreasing the Si/Al ratio, the total selectivity to C11 and C12 hydrocarbons decreased, while the total selectivity to isoundecane and isododecane (Si-C11+i-C12) firstly increased and then decreased. Ni2P/AlMCM-41-5 gave the largest Si-C11+i-C12 of 43.2%. While NiP/AlMCM-41-5-TPR gave higher Si-C11+i-C12 than Ni2P/AlMCM-41-5, it was more active for the undesired Csbnd C bond cleavage and methanation. We propose that the in-situ phosphorization adopted here is a promising approach to preparing Ni2P-based bifunctional catalysts.

  5. Performance of La,Ce-modified alumina-supported Pt and Ni catalysts for the oxidative reforming of diesel hydrocarbons

    Energy Technology Data Exchange (ETDEWEB)

    Alvarez-Galvan, M.C.; Navarro, R.M.; Fierro, J.L.G. [Instituto de Catalisis y Petroleoquimica (CSIC), Marie Curie 2, Cantoblanco E-28049, Madrid (Spain); Rosa, F. [Centro de Experimentacion de ' ' El Arenosillo' ' (CEDEA), Instituto Nacional de Tecnica Aeroespacial (INTA), E- 21130 Mazagon-Moguer, Huelva (Spain); Briceno, Y. [CIDAUT, Parque Tecnologico Boecillo, Valladolid (Spain); Gordillo Alvarez, F. [Escuela Superior de Ingenieros, Sevilla (Spain)

    2008-01-15

    Platinum and nickel phases deposited on alumina modified with lanthanum and cerium oxides have been used in the oxidative reforming of hexadecane, decalin and tetralin, hydrocarbons selected as surrogates for the paraffin, cycloparaffin and aromatic fractions present in diesel fuel. Activity results showed that reforming capacity depends on the type of active phase as well as on the reactant molecule. Ni catalyst recorded a greater hydrogen production than Pt counterpart for all feeds. The higher activity for decalin is attributed to the more labile tertiary carbons of this molecule, and the lower activity for tetralin, to the higher bond dissociation energy of the aromatic C-C and C-H bonds. The characterization results (obtained by TPR and XPS) revealed a greater active metal-ceria interface in Ni catalyst which may have a role regarding its better catalytic performance and higher intrinsic activity for hydrogen production, as well as the lesser coke deposition. (author)

  6. Development of Fe-Ni/YSZ-GDC electro-catalysts for application as SOFC anodes. XRD and TPR characterization, and evaluation in ethanol steam reforming reaction

    Energy Technology Data Exchange (ETDEWEB)

    Paz Fiuza, Raigenis da; Silva, Marcos Aurelio da; Boaventura, Jaime Soares [UFBA, Salvador, Bahia (Brazil). Energy and Materials Science Group

    2010-07-01

    Electro-catalysts based on Fe-Ni alloys were prepared using physical mixture and modified Pechini methods; they were supported on a composite of Yttria Stabilized Zirconia (YSZ) and Gadolinia Doped Ceria (GDC). The composites had compositions of 35% metal load and 65% support (70% wt. YSZ and 30% wt. GDC mixture) (cermets). The samples were characterized by Temperature-Programmed Reduction (TPR) and X-Ray Diffraction (XRD) and evaluated in ethanol steam reforming at 650 C for six hours and in the temperature range 300 - 900 C. The XRD results showed that the bimetallic sample calcined at 800 C formed a mixed oxide (NiFe{sub 2}O{sub 4}) in spinel structure; after reducing the sample in hydrogen, Ni-Fe alloys were formed. The presence of Ni decreased the final reduction temperature of the NiFe{sub 2}O{sub 4} species. The addition of Fe to Ni anchored to YSZ-GDC increased the hydrogen production and inhibits the carbon deposition. The bimetallic 30Fe5Ni samples reached an ethanol conversion of about 95%, and a hydrogen yield up to 48% at 750 C. In general, the ethanol conversion and hydrogen production were independent of the metal content in the electro-catalyst. However, the substitution of Ni for Fe significantly reduced the carbon deposition on the electro-catalyst: 74, 31 and 9 wt. % in the 35Ni, 20Fe15Ni, and 30Fe5Ni samples, respectively. (orig.)

  7. Pyrolysis and gasification of landfilled plastic wastes with Ni-Mg-La/Al2O3 catalyst.

    Science.gov (United States)

    Kaewpengkrow, Prangtip; Atong, Duangduen; Sricharoenchaikul, Viboon

    2012-12-01

    Pyrolysis and gasification processes were utilized to study the feasibility of producing fuels from landfilled plastic wastes. These wastes were converted in a gasifier at 700-900 degrees C. The equivalence ratio (ER) was varied from 0.4-0.6 with or without addition ofa Ni-Mg-La/Al2O3 catalyst. The pyrolysis and gasification of plastic wastes without catalyst resulted in relatively low H2, CO and other fuel gas products with methane as the major gaseous species. The highest lower heating value (LHV) was obtained at 800 degrees C and for an ER of 0.4, while the maximum cold gas efficiency occurred at 700 degrees C and for an ER of 0.4. The presence of the Ni-Mg-La/Al2O3 catalyst significantly enhanced H2 and CO production as well as increasing the gas energy content to 15.76-19.26 MJ/m3, which is suitable for further usage as quality fuel gas. A higher temperature resulted in more H2 and CO and other product gas yields, while char and liquid (tars) decreased. The maximum gas yield, gas calorific value and cold gas efficiency were achieved when the Ni-Mg-La/Al2O3 catalyst was used at 900 degrees C. In general, addition of prepared catalyst resulted in greater H2, CO and other light hydrocarbon yields from superior conversion of wastes to these gases. Thus, thermochemical treatment of these problematic wastes using pyrolysis and gasification processes is a very attractive alternative for sustainable waste management.

  8. A Non-sulfided flower-like Ni-PTA Catalyst that Enhances the Hydrotreatment Efficiency of Plant Oil to Produce Green Diesel

    Science.gov (United States)

    Liu, Jing; Chen, Pan; Deng, Lihong; He, Jing; Wang, Luying; Rong, Long; Lei, Jiandu

    2015-01-01

    The development of a novel non-sulfided catalyst with high activity for the hydrotreatment processing of plant oils, is of high interest as a way to improve the efficient production of renewable diesel. To attempt to develop such a catalyst, we first synthesized a high activity flower-like Ni-PTA catalyst used in the hydrotreatment processes of plant oils. The obtained catalyst was characterized with SEM, EDX, HRTEM, BET, XRD, H2-TPR, XPS and TGA. A probable formation mechanism of flower-like Ni(OH)2 is proposed on the basis of a range of contrasting experiments. The results of GC showed that the conversion yield of Jatropha oil was 98.95%, and the selectivity of C11-C18 alkanes was 70.93% at 360 °C, 3 MPa, and 15 h−1. The activity of this flower-like Ni-PTA catalyst was more than 15 times higher than those of the conventional Ni-PTA/Al2O3 catalysts. Additionally, the flower-like Ni-PTA catalyst exhibited good stability during the process of plant oil hydrotreatment. PMID:26503896

  9. Catalytic reforming of toluene as tar model compound: effect of Ce and Ce-Mg promoter using Ni/olivine catalyst.

    Science.gov (United States)

    Zhang, Ruiqin; Wang, Huajian; Hou, Xiaoxue

    2014-02-01

    Tar produced by biomass gasification as a route of renewable energy must be removed before the gas can be used. This study was undertaken using toluene as a model tar compound for evaluating its steam reforming conversion with three Ni-based catalysts, Ni/olivine, Ni-Ce/olivine and Ni-Ce-Mg/olivine. Effects of Ce and Mg promoters on the reaction activity and coke deposition were studied. Overall the performance of Ce and Mg promoted Ni/olivine catalysts is better than that of only Ce promoter and Ni/olivine alone. The experimental results indicate that Ni-Ce-Mg/olivine catalysts could improve the resistance to carbon deposition, enhance energy gases yield and resist 10ppm H2S poison at 100mLmin(-1) for up to 400min. Furthermore, the activity of catalysts was related to the steam/carbon (S/C) ratios; at S/C ratio=5, T=790°C, space velocity=782h(-1) and t=2h, the Ni-Ce-Mg/olivine system yielded 89% toluene conversion, 5.6Lh(-1) product gas rate, 62.6mol% H2 content and 10% (mol useful gas mol(-1) toluene) energy yield. Moreover, at low S/C ratio, it had higher reaction activity and better ability to prevent coking. There is a small amount of carbon deposition in the form of amorphous carbon after 7h. Various characterization techniques such as XRD, FTIR and thermogravimetric were performed to investigate the coke deposition of Ni/olivine, Ni-Ce/olivine and Ni-Ce-Mg/olivine. It is suggested that 3% Ni-1% Ce-1% Mg/olivine was the most promising catalyst due to its minimum coke amount and the lower activation energy of coke burning. Copyright © 2014. Published by Elsevier Ltd.

  10. A comparative study of alumina-supported Ni catalysts prepared by photodeposition and impregnation methods on the catalytic ozonation of 2,4-dichlorophenoxyacetic acid

    Energy Technology Data Exchange (ETDEWEB)

    Rodríguez, Julia L., E-mail: ozliliana@yahoo.com.mx [Lab. Ing. Química Ambiental. ESIQIE–Instituto Politécnico Nacional (Mexico); Valenzuela, Miguel A. [Lab.Catálisis y Materiales. ESIQIE–Instituto Politécnico Nacional. Zacatenco (Mexico); Tiznado, Hugo [Centro de Nanociencias y Nanotecnología. CNyN Universidad Nacional Autónoma de México (Mexico); Poznyak, Tatiana [Lab. Ing. Química Ambiental. ESIQIE–Instituto Politécnico Nacional (Mexico); Chairez, Isaac [Departamento de Bioprocesos, UPIBI- Instituto Politécnico Nacional (Mexico); Magallanes, Diana [Lab. Ing. Química Ambiental. ESIQIE–Instituto Politécnico Nacional (Mexico)

    2017-02-15

    The heterogeneous catalytic ozonation on unsupported and supported oxides has been successfully tested for the removal of several refractory compounds in aqueous solution. In this work, alumina-supported nickel catalysts prepared by photodeposition and impregnation methods were compared in the catalytic ozonation of 2,4-dichlorophenoxyacetic acid (2,4-D). The catalysts were characterized by high-resolution electron microscopy and X-ray photoelectron spectroscopy. The photochemical decomposition of Ni acetylacetonate to produce Ni(OH){sub 2}, NiO, and traces of Ni° deposited on alumina was achieved in the presence of benzophenone as a sensitizer. A similar surface composition was found with the impregnated catalyst after its reduction with hydrogen at 500 °C and exposed to ambient air. Results indicated a higher initial activity and maleic acid (byproduct) concentration with the photodeposited catalyst (1 wt% Ni) compared to the impregnated catalyst (3 wt% Ni). These findings suggest the use of the photodeposition method as a simple and reliable procedure for the preparation of supported metal oxide/metal catalysts under mild operating conditions.

  11. Steam Reforming of Ethylene Glycol over Ni/Al{sub 2}O{sub 3} Catalysts: Effect of the Preparation Method and Reduction Temperature

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Dong Hyuck; Park, Jung Eun; Park, Eun Duck [Ajou University, Suwon (Korea, Republic of)

    2015-02-15

    The effect of preparation method on the catalytic activities of the Ni/Al{sub 2}O{sub 3} catalysts on steam reforming of ethylene glycol was investigated. The catalysts were prepared with various preparation methods such as an incipient wetness impregnation, wet impregnation, and coprecipitation method. In the case of coprecipitation method, various precipitants such as KOH, K{sub 2}CO{sub 3}, and NH{sub 4}OH were compared. The prepared catalysts were characterized by using N{sub 2} physisorption, inductively coupled plasma-atomic emission spectroscopy, X-ray diffraction, temperature programmed reduction, pulsed H{sub 2} chemisorption, temperature-programmed oxidation, scanning electron microscopy, and thermogravimetric analysis. Among the catalysts reduced at 773 K, the Ni/Al{sub 2}O{sub 3} catalyst prepared by a coprecipitation with KOH or K{sub 2}CO{sub 3} as precipitants showed the best catalytic performance. The preparation method affected the particle size of Ni, reducibility of nickel oxides, catalytic performance (activity and stability), and types of coke formed during the reaction. The Ni/Al{sub 2}O{sub 3} catalyst prepared by a coprecipitation with KOH showed the increasing catalytic activity with an increase in the reduction temperature from 773 to 1173 K because of an increase in the reduction degree of Ni oxide species even though the particle size of Ni increased with increasing reduction temperature.

  12. Steam reforming of biomass tar producing H2-rich gases over Ni/MgOx/CaO1-x catalyst.

    Science.gov (United States)

    Li, Chunshan; Hirabayashi, Daisuke; Suzuki, Kenzi

    2010-01-01

    Series nickel catalysts Ni/MgO(x)/CaO(1-)(x) (x=0.3, 0.5, 0.7, Ni: 5 wt%) were prepared and tested in fixed-bed reactor for biomass tar steam reforming, toluene as tar destruction model compound. Different ratios of MgO and CaO were mixed to simulate dolomite as Ni support. Two preparation methods: solid mixing with (SMW) and without water (SM) were used, the preparation methods and concentration of MgO had an important influence on toluene conversion and products. Catalysts prepared by SM method exhibited higher performance on toluene conversion, resulted in higher H(2) yield, and also, higher CO(2) and lower CO selectivity with higher temperature. For the same preparation method, higher concentration of MgO resulted in higher toluene conversion, and also influence on CO, CO(2) selectivity, but no obvious influence on the H(2) yield. Catalysts were characterized by BET, X-ray diffraction (XRD), SEM.

  13. Phase-Contact Engineering in Mono- and Bimetallic Cu-Ni Co-catalysts for Hydrogen Photocatalytic Materials.

    Science.gov (United States)

    Muñoz-Batista, Mario J; Motta Meira, Debora; Colón, Gerardo; Kubacka, Anna; Fernández-García, Marcos

    2018-01-26

    Understanding how a photocatalyst modulates its oxidation state, size, and structure during a photocatalytic reaction under operando conditions is strongly limited by the mismatch between (catalyst) volume sampled by light and, to date, the physicochemical techniques and probes employed to study them. A synchrotron micro-beam X-ray absorption spectroscopy study together with the computational simulation and analysis (at the X-ray cell) of the light-matter interaction occurring in powdered TiO2 -based monometallic Cu, Ni and bimetallic CuNi catalysts for hydrogen production from renewables was carried out. The combined information unveils an unexpected key catalytic role involving the phase contact between the reduced and oxidized non-noble metal phases in all catalysts and, additionally, reveals the source of the synergistic Cu-Ni interaction in the bimetallic material. The experimental method is applicable to operando studies of a wide variety of photocatalytic materials. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. 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.

  15. Session 4: Carbon dioxide reforming of methane over Ni/Al{sub 2}O{sub 3} catalysts - a new activation process

    Energy Technology Data Exchange (ETDEWEB)

    Souza, M.M.V.M. de; Perez, C.A.C.; Schmal, M. [Rio de Janeiro Univ., NUCAT/PEQ/COPPE (Brazil); Clave, L.; Dubois, V. [Institut Meurice Brussels (Belgium)

    2004-07-01

    The aim of this work is to investigate the role of a new activation, in which the catalyst is treated by a CH{sub 4}/O{sub 2} stream, over the activity and stability of Ni/Al{sub 2}O{sub 3} catalysts for CO{sub 2} reforming of methane. The obtained experimental results are explained. (O.M.)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-09-01

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

  17. The effect of noble metals on catalytic methanation reaction over supported Mn/Ni oxide based catalysts

    Directory of Open Access Journals (Sweden)

    Wan Azelee Wan Abu Bakar

    2015-09-01

    Full Text Available Carbon dioxide (CO2 in sour natural gas can be removed using green technology via catalytic methanation reaction by converting CO2 to methane (CH4 gas. Using waste to wealth concept, production of CH4 would increase as well as creating environmental friendly approach for the purification of natural gas. In this research, a series of alumina supported manganese–nickel oxide based catalysts doped with noble metals such as ruthenium and palladium were prepared by wetness impregnation method. The prepared catalysts were run catalytic screening process using in-house built micro reactor coupled with Fourier Transform Infra Red (FTIR spectroscopy to study the percentage CO2 conversion and CH4 formation analyzed by GC. Ru/Mn/Ni(5:35:60/Al2O3 calcined at 1000 °C was found to be the potential catalyst which gave 99.74% of CO2 conversion and 72.36% of CH4 formation at 400 °C reaction temperature. XRD diffractogram illustrated that the supported catalyst was in polycrystalline with some amorphous state at 1000 °C calcination temperature with the presence of NiO as active site. According to FESEM micrographs, both fresh and used catalysts displayed spherical shape with small particle sizes in agglomerated and aggregated mixture. Nitrogen Adsorption analysis revealed that both catalysts were in mesoporous structures with BET surface area in the range of 46–60 m2/g. All the impurities have been removed at 1000 °C calcination temperature as presented by FTIR, TGA–DTA and EDX data.

  18. Catalytic Hydrogenation of Levulinic Acid in Water into g-Valerolactone over Bulk Structure of Inexpensive Intermetallic Ni-Sn Alloy Catalysts

    Directory of Open Access Journals (Sweden)

    Rodiansono Rodiansono

    2015-07-01

    Full Text Available A bulk structure of inexpensive intermetallic nickel-tin (Ni-Sn alloys catalysts demonstrated highly selective in the hydrogenation of levulinic acid in water into g-valerolactone. The intermetallic Ni-Sn catalysts were synthesized via a very simple thermochemical method from non-organometallic precursor at low temperature followed by hydrogen treatment at 673 K for 90 min. The molar ratio of nickel salt and tin salt was varied to obtain the corresponding Ni/Sn ratio of 4.0, 3.0, 2.0, 1.5, and 0.75. The formation of Ni-Sn alloy species was mainly depended on the composition and temperature of H2 treatment. Intermetallics Ni-Sn that contain Ni3Sn, Ni3Sn2, and Ni3Sn4 alloy phases are known to be effective heterogeneous catalysts for levulinic acid hydrogenation giving very excellence g-valerolactone yield of >99% at 433 K, initial H2 pressure of 4.0 MPa within 6 h. The effective hydrogenation was obtained in H2O without the formation of by-product. Intermetallic Ni-Sn(1.5 that contains Ni3Sn2 alloy species demonstrated very stable and reusable catalyst without any significant loss of its selectivity. © 2015 BCREC UNDIP. All rights reserved. Received: 26th February 2015; Revised: 16th April 2015; Accepted: 22nd April 2015  How to Cite: Rodiansono, R., Astuti, M.D., Ghofur, A., Sembiring, K.C. (2015. Catalytic Hydrogenation of Levulinic Acid in Water into g-Valerolactone over Bulk Structure of Inexpensive Intermetallic Ni-Sn Alloy Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 10 (2: 192-200. (doi:10.9767/bcrec.10.2.8284.192-200Permalink/DOI: http://dx.doi.org/10.9767/bcrec.10.2.8284.192-200  

  19. Transfer hydrogenation of olefin from alcohol using a hydrogen-absorbing alloy (CaNi{sub 5}) catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Imamura, H.; Tanaka, T.; Sakata, Y.; Tsuchiya, S. [Yamaguchi Univ., Ube (Japan). Faculty of Engineering

    1999-12-20

    Gas-phase reactions between 2-butene and 2-propanol on a hydrogen-absorbing alloy CaNi{sub 5} have been studied in the temperature range of 393 to 473 K. CaNi{sub 5} showed interesting characteristics as an active catalyst for the transfer hydrogenation of butene from propanol as a hydrogen donor. 2-Propanol was effectively dehydrogenated to yield acetone, in which the dissociated hydrogen was completely absorbed by CaNi{sub 5} to form the metal hydride. When the alloy was hydrided to some extent, butene was effectively hydrogenated by the absorbed hydrogen in the metal hydride to produce butane. The overall reaction was expressed as catalytic transfer hydrogenation through the formation of metal hydride intermediates (CaNi{sub 5}H{sub n}). Catalytic transfer hydrogenation on CaNi{sub 5} occurred at 423 K via hydriding of CaNi{sub 5} by 2-propanol dehydrogenation with subsequent dehydriding for the hydrogenation of 2-butene, rather than the direct reaction between 2-butene and 2-propanol on the alloy. (orig.)

  20. Location and coordination of promoter atoms in Co- and Ni-promoted MoS2-based hydrotreating catalysts

    DEFF Research Database (Denmark)

    Lauritsen, Jeppe V.; Kibsgaard, Jakob; Olesen, Georg H.

    2007-01-01

    on the nanocluster size. Larger clusters (type A) are structurally similar to Co–Mo–S exposing fully Ni-substituted (1010) edges with a 50% S coverage. Smaller clusters (type B) show dodecagonal shapes terminated by three different edges, all of which contain Ni-promoter atoms fully or partially substituting the Mo......In this study, we used scanning tunneling microscopy (STM) and density functional theory (DFT) to investigate the atomic-scale structure of the active Co- or Ni-promoted MoS2 nanoclusters in hydrotreating catalysts. Co-promoted MoS2 nanoclusters (Co–Mo–S) are found to adopt a hexagonal shape......, with Co atoms preferentially located at (1010) edges with a 50% sulfur coverage. The first atom-resolved STM images of the Ni-promoted MoS2 nanoclusters (Ni–Mo–S) reveal that the addition of Ni also leads to truncated morphologies, but the degree of truncation and the Ni sites are observed to depend...

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

    African Journals Online (AJOL)

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

  2. Cuboid Ni2P as a Bifunctional Catalyst for Efficient Hydrogen Generation from Hydrolysis of Ammonia Borane and Electrocatalytic Hydrogen Evolution.

    Science.gov (United States)

    Du, Yeshuang; Liu, Chao; Cheng, Gongzhen; Luo, Wei

    2017-11-16

    The design of high-performance catalysts for hydrogen generation is highly desirable for the upcoming hydrogen economy. Herein, we report the colloidal synthesis of nanocuboid Ni 2 P by the thermal decomposition of nickel chloride hexahydrate (NiCl 2 ⋅6 H 2 O) and trioctylphosphine. The obtained nanocuboid Ni 2 P was characterized by using powder X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and inductively coupled plasma atomic emission spectroscopy. For the first time, the as-synthesized nanocuboid Ni 2 P is used as a bifunctional catalyst for hydrogen generation from the hydrolysis of ammonia borane and electrocatalytic hydrogen evolution. Owing to the strong synergistic electronic effect between Ni and P, the as-synthesized Ni 2 P exhibits catalytic performance that is superior to its counterpart without P doping. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. The influence of Ni load and support material on catalysts for the selective catalytic oxidation of ammonia in gasified biomass

    Energy Technology Data Exchange (ETDEWEB)

    Nassos, S.; Elm Svensson, E.; Boutonnet, M.; Jaeraas, S.G. [KTH Royal Institute of Technology, Chemical Engineering and Technology, Chemical Technology, Teknikringen 42, S-10044 Stockholm (Sweden)

    2007-06-18

    The effect of nickel (Ni) load (0, 5 and 10 wt.%) and support material (Ce{sub 0.9}La{sub 0.1}O{sub 2}, Ce{sub 0.9}Zr{sub 0.1}O{sub 2} and {gamma}-Al{sub 2}O{sub 3}), together the amount of oxygen ({lambda} = 0.25 and {lambda} = 0.5) and gas hourly space velocity (50 000, 100 000 and 150 000 h{sup -1}) were investigated for the selective catalytic oxidation of ammonia in gasified biomass. The mixed metal oxide support materials were prepared by microemulsion, whereas the alumina was a commercial product. Ni was added to the different supports by incipient wetness. All the obtained catalysts were characterised by BET and XRD analysis. Cordierite monoliths coated with 20 wt.% catalytic material were tested in a tubular quartz reactor. For simulating the gasified biomass fuel, 500 ppm of NH{sub 3} was added to the fuel. Water was also present during the activity tests, which were carried out between 500 and 750 C. The results from the activity tests at {lambda} = 0.25 and gas hourly space velocity of 100 000 h{sup -1} indicated that the 10 wt.% Ni on Ce{sub 0.9}La{sub 0.1}O{sub 2} was the best catalyst obtaining 65 and 97% N{sub 2} yield at 500 and 750 C, respectively. By increasing {lambda} to 0.5 and decreasing the gas hourly space velocity, the N{sub 2} yield improved considerably at low temperature level (500 C). Moreover, NO{sub x} emissions maintained at low levels depending on the experimental conditions. Constant conversion and negligible carbon deposition were also two other important observations from the mixed metal oxide supported catalysts. On the contrary, all the alumina-based catalysts displayed the lowest performance. (author)

  4. Ni3 FeN-Supported Fe3 Pt Intermetallic Nanoalloy as a High-Performance Bifunctional Catalyst for Metal-Air Batteries.

    Science.gov (United States)

    Cui, Zhiming; Fu, Gengtao; Li, Yutao; Goodenough, John B

    2017-08-07

    Electrocatalysts for both the oxygen reduction and evolution reactions (ORR and OER) are vital for the performances of rechargeable metal-air batteries. Herein, we report an advanced bifunctional oxygen electrocatalyst consisting of porous metallic nickel-iron nitride (Ni3 FeN) supporting ordered Fe3 Pt intermetallic nanoalloy. In this hybrid catalyst, the bimetallic nitride Ni3 FeN mainly contributes to the high activity for the OER while the ordered Fe3 Pt nanoalloy contributes to the excellent activity for the ORR. Robust Ni3 FeN-supported Fe3 Pt catalysts show superior catalytic performance to the state-of-the-art ORR catalyst (Pt/C) and OER catalyst (Ir/C). The Fe3 Pt/Ni3 FeN bifunctional catalyst enables Zn-air batteries to achieve a long-term cycling performance of over 480 h at 10 mA cm-2 with high efficiency. The extraordinarily high performance of the Fe3 Pt/Ni3 FeN bifunctional catalyst makes it a very promising air cathode in alkaline electrolyte. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  5. Influence of excess sodium ions on the specific surface area formation in a NiO-Al2O3 catalyst prepared by different methods

    Directory of Open Access Journals (Sweden)

    Lazić M.M.

    2008-01-01

    Full Text Available The influence of sodium ions on the specific surface area of a NiO-Al2O3 catalyst in dependence of nickel loading (5, 10, and 20 wt% Ni, temperature of heat treatment (400, 700 and 1100oC and the method of sample preparation was investigated. Low temperature nitrogen adsorption (LTNA, X-ray diffraction (XRD and scanning electron microscopy (SEM were applied for sample characterization. Dramatic differences in the specific surface area were registered between non-rinsed and rinsed Al2O3 and NiO-Al2O3 samples. The lagged sodium ions promote sintering of non-rinsed catalyst samples.

  6. Use of Ni-Zn ferrites doped with Cu as catalyst in the transesterification of soybean oil to methyl esters

    Energy Technology Data Exchange (ETDEWEB)

    Dantas, Joelda; Santos, Jakeline Raiane D.; Cunha, Rodrigo Bruno L.; Costa, Ana Cristina F.M., E-mail: joeldadantas@yahoo.com.br [Universidade Federal de Campina Grande (LabSMaC/UFCG), PB (Brazil). Dept. de Engenharia de Materiais. Lab. de Sintese de Materiais Ceramicos; Kiminami, Ruth Herta G.A. [Universidade Federal de Sao Carlos (UFSCar), SP (Brazil). Dept. de Engenhria de Materiais

    2013-11-01

    The purpose of this work is to evaluate the performance of Ni{sub 0.5}Zn{sub 0.5}Fe{sub 2}O{sub 4} ferrite doped with 0.1 and 0.4 mol of Cu as a catalyst for the transesterification of soybean oil to biodiesel, using methanol. The samples were characterized by X-ray diffraction, nitrogen adsorption and scanning electron microscopy. The reaction was performed for 2 hours at a temperature of 160 Degree-Sign C, using 10 g of soybean oil, a molar ratio of oil: alcohol of 1:20, and 4% (w/w) of catalyst. The product of the reaction was characterized by gas chromatography, which confirmed conversion to methyl esters. The diffraction patterns showed the presence only of Ni{sub 0.5}Zn{sub 0.5}Fe{sub 2}O{sub 4} ferrite phase with a crystallite size of 29 nm. The samples doped with 0.1 and 0.4 mol of Cu showed a surface area and particle size of 22.17 {sup m2}g{sup -1} and 50.47 nm; and 23.49 m{sup 2}g{sup -1} and 47.64 nm, respectively. The morphology of both samples consisted of brittle block-shaped agglomerates with a wide particle size distribution. A comparative analysis of the two catalysts indicated that the catalyst doped with 0.4 mol of Cu showed the better performance, with a conversion rate of 50.25%, while the catalyst doped with 0.1 mol of Cu showed 42.71% conversion. (author)

  7. Use of Ni-Zn ferrites doped with Cu as catalyst in the transesterification of soybean oil to methyl esters

    Directory of Open Access Journals (Sweden)

    Joelda Dantas

    2013-06-01

    Full Text Available The purpose of this work is to evaluate the performance of Ni0.5Zn0.5Fe2O4 ferrite doped with 0.1 and 0.4 mol of Cu as a catalyst for the transesterification of soybean oil to biodiesel, using methanol. The samples were characterized by X-ray diffraction, nitrogen adsorption and scanning electron microscopy. The reaction was performed for 2 hours at a temperature of 160 °C, using 10 g of soybean oil, a molar ratio of oil: alcohol of 1:20, and 4% (w/w of catalyst. The product of the reaction was characterized by gas chromatography, which confirmed conversion to methyl esters. The diffraction patterns showed the presence only of Ni0.5Zn0.5Fe2O4 ferrite phase with a crystallite size of 29 nm. The samples doped with 0.1 and 0.4 mol of Cu showed a surface area and particle size of 22.17 m²g- 1 and 50.47 nm; and 23.49 m²g- 1 and 47.64 nm, respectively. The morphology of both samples consisted of brittle block-shaped agglomerates with a wide particle size distribution. A comparative analysis of the two catalysts indicated that the catalyst doped with 0.4 mol of Cu showed the better performance, with a conversion rate of 50.25%, while the catalyst doped with 0.1 mol of Cu showed 42.71% conversion.

  8. Comparison between Ni-Rh/gadolinia doped ceria catalysts in reforming of propane for anode implementations in intermediate solid oxide fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Boaro, M.; Pappacena, A. [Universita di Udine, Dipartimento di Scienze e Tecnologie Chimiche, via Cotonificio 108, 33100 Udine (Italy); Modafferi, V.; Frontera, P. [Universita Mediterranea, Dipartimento Meccanica e Materiali, Feo di Vito, 89060 Reggio Calabria (Italy); Llorca, J. [Institut de Tecniques Energetiques, Universitat Politecnica de Catalunya, Diagonal 647, ed. ETSEIB, 08028 Barcelona (Spain); Baglio, V.; Frusteri, F. [CNR-ITAE ' ' Nicola Giordano' ' , Salita S. Lucia 5, 98126 Messina (Italy); Trovarelli, A. [Universita di Udine, Dipartimento di Scienze e Tecnologie Chimiche, via Cotonificio 108, 33100 Udine (Italy); INSTM-Consorzio Interuniversitario Nazionale per le Scienze e Tecnologie dei Materiali, via Giusti 9, 50121 Firenze (Italy); Antonucci, P.L. [Universita Mediterranea, Dipartimento Meccanica e Materiali, Feo di Vito, 89060 Reggio Calabria (Italy); INSTM-Consorzio Interuniversitario Nazionale per le Scienze e Tecnologie dei Materiali, via Giusti 9, 50121 Firenze (Italy)

    2010-01-15

    Steam and autothermal reforming of propane over Ni-Rh/GDC catalysts prepared by coprecipitation and by Pechini method were investigated in the temperature range 873-1073 K. The weight ratio for Ni, Rh and Ce{sub 0.8}Gd{sub 0.2}O{sub 2} (45:5:50) and the operating temperatures were chosen in order to gain propaedeutical information on fuel reactivity under typical intermediate solid oxide fuel cell (IT-SOFC) operating conditions. The Pechini synthesis allows to obtain catalysts with lower surface area, smaller nickel crystallites and a bimodal distribution of rhodium in comparison to the coprecipitation method. Despite the different methods of synthesis lead to catalysts with different morphological and structural properties, the activity of catalysts is quite similar. At reaction temperature higher than 973 K, under both steam reforming (SR) and autothermal reforming (ATR), the catalysts show high propane conversion and syngas (H{sub 2} + CO) productivity. Deactivation of catalysts was observed at 873 and 973 K under SR conditions due to coke formation. In ATR, coke formation was almost completely depressed and the catalysts resulted to be very stable even at low reaction temperature (873 K). In SR coke formation occurs with higher rate on the catalyst having higher Ni dispersion, probably since propane cracking reaction is the pre-eminent phenomenon in promoting coke formation. (author)

  9. Catalisadores Ni/Al2O3 promovidos com molibdênio para a reação de reforma a vapor de metano Mo-Ni/AL2O3 catalysts for the methane steam reforming reaction

    Directory of Open Access Journals (Sweden)

    Silvia Sálua Maluf

    2003-03-01

    Full Text Available Mo-promoted Ni/Al2O3 catalysts for the methane steam reforming reaction were studied in this work. The Ni/Al2O3 catalysts were prepared by precipitation and molibdenum was added by impregnation up to 2%wt. The solids were tested using a micro-reactor under two H2Ov/C conditions and were characterized by ICP-OES, XRD, N2 adsoption, H2 chemisorption and TPR. NiO and NiAl2O4 phases were observed and the metallic area decreased with the increase of the Mo content. From the catalytic tests high stability was verified for H2Ov/C=4.0. On the other hand, only the catalyst containing 0,05% Mo stayed stable during 30 hours of the test at H2Ov/C=2.0.

  10. Probing the electronic structure of M-graphene oxide (M = Ni, Co, NiCo) catalysts for hydrolytic dehydrogenation of ammonia borane

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, Binhua; Liu, Jinyin; Zhou, Litao [Soochow University-Western University Centre for Synchrotron Radiation Research, Institute of Functional Nano and Soft Material (FUNSOM) and Collaborative Innovation Center of Suzhou Nano Science & Technology, Soochow University, Suzhou 215123 (China); Long, Dan, E-mail: legend_long@aliyun.com [Department of Radiology, Zhejiang Cancer Hospital, Hangzhou 310022 (China); Feng, Kun; Sun, Xuhui [Soochow University-Western University Centre for Synchrotron Radiation Research, Institute of Functional Nano and Soft Material (FUNSOM) and Collaborative Innovation Center of Suzhou Nano Science & Technology, Soochow University, Suzhou 215123 (China); Zhong, Jun, E-mail: jzhong@suda.edu.cn [Soochow University-Western University Centre for Synchrotron Radiation Research, Institute of Functional Nano and Soft Material (FUNSOM) and Collaborative Innovation Center of Suzhou Nano Science & Technology, Soochow University, Suzhou 215123 (China)

    2016-01-30

    Graphical abstract: An interaction between metal and graphene oxide was probed to enhance the hydrolysis efficiency of ammonia borane. - Highlights: • Various metal elements (M = Ni, Co, NiCo) were dispersed on graphene oxide (GO) for the hydrolysis of ammonia borane (AB). • The electronic structure of the hybrids has been probed by scanning transmission X-ray microscopy (STXM). • An interfacial interaction between metal and GO was observed which could be related to the hydrolysis performance. • The results provide new insight into the enhanced performance of the M-GO hybrids. - Abstract: Various metal elements (M = Ni, Co, NiCo) were dispersed on graphene oxide (GO) to form the M-GO hybrids by a facile way. The hybrids showed good catalytic activities in the hydrolytic dehydrogenation of ammonia borane (AB, NH{sub 3}BH{sub 3}), which were significantly enhanced when compared to the metal nanoparticles or GO alone. The electronic structure of the hybrids has been probed by scanning transmission X-ray microscopy (STXM). The distribution of metal elements was clearly imaged with identical electronic structure. Moreover, an interfacial interaction between metal and GO was observed with the peak intensity proportional to the catalytic performance in the hydrolysis of AB. The results provide new insight into the enhanced performance of the M-GO hybrids and may help for the design of advanced catalysts.

  11. Oxidation Kinetics of Propane-Air Mixture over NiCo2O4 Catalyst Emitted from LPG Vehicles

    Directory of Open Access Journals (Sweden)

    Suverna Trivedi

    2017-05-01

    Full Text Available This paper describes the kinetics of catalytic air oxidation of propane. The kinetics data were collected in a plug flow tubular reactor. The experiments were performed over the NiCo2O4 catalyst prepared by co-precipitation method followed by calcination at 400 oC. The kinetic data were collected under the following conditions: 200 mg of catalyst, 2.5 % of propane in air, total flow rate of 60 mL/min, and temperature ranges of 130-170 oC. The data were fitted to the power law rate equation. The activation    energy and frequency factor were found to be 59.3 kJ/g mol and 2.9×108 (mol0.47.L0.53/g cat.h, respectively. Copyright © 2017 BCREC Group. All rights reserved Received: 20th November 2016; Revised: 26th February 2017; Accepted: 26th February 2017 How to Cite: Trivedi, S., Prasad, R., Chadha, S. (2017. Oxidation Kinetics of Propane-Air Mixture over NiCo2O4 Catalyst Emitted from LPG Vehicles. Bulletin of Chemical Reaction Engineering & Catalysis, 12 (2: 191-196 (doi:10.9767/bcrec.12.2.798.191-196 Permalink/DOI: http://dx.doi.org/10.9767/bcrec.12.2.798.191-196

  12. Model bimetallic Pd-Ni automotive exhaust catalysts. Influence of thermal aging and hydrocarbon self-poisoning

    Energy Technology Data Exchange (ETDEWEB)

    Hungria, A.B.; Martinez-Arias, A. [Instituto de Catalisis y Petroleoquimica, CSIC, C/Marie Curie 2, Campus Cantoblanco, 28049 Madrid (Spain); Calvino, J.J. [Dpto. de Ciencia de los Materiales e Ingenieria Metalurgica y Quimica Inorganica, Facultad de Ciencias, Universidad de Cadiz, 11510 Puerto Real, Cadiz (Spain); Anderson, J.A. [Surface Chemistry and Catalysis Group, Department of Chemistry, University of Aberdeen, AB24 3UE Scotland (United Kingdom)

    2006-02-22

    Bimetallic Pd-Ni catalysts supported on Al{sub 2}O{sub 3} and (Ce,Zr)O{sub x}/Al{sub 2}O{sub 3} were examined with respect to their catalytic performance for the elimination of CO, NO and C{sub 3}H{sub 6} under stoichiometric conditions. The effects of a thermal aging treatment at 1273K, reactant competition in the presence of the hydrocarbon and the influence of the presence of nickel in the catalyst have been analysed by XRD, HREM, catalytic activity measurements and in situ DRIFTS spectroscopy. Self-poisoning effects, induced by the presence of the hydrocarbon in the reactant mixture, were identified as the main factor affecting the light-off activity. While a Ni-induced preferential interaction between Pd and the Ce-Zr mixed oxide component appears, in general terms, to be beneficial for the catalytic performance of the fresh (Ce,Zr)O{sub x}/Al{sub 2}O{sub 3}-supported bimetallic catalyst, it is shown to be detrimental for the aged system as a consequence of a facilitated degradation of the (Ce,Zr)O{sub x} component and encapsulation of the active palladium particles. (author)

  13. Room temperature hydrogen generation from hydrolysis of ammonia-borane over an efficient NiAgPd/C catalyst

    KAUST Repository

    Hu, Lei

    2014-12-01

    NiAgPd nanoparticles are successfully synthesized by in-situ reduction of Ni, Ag and Pd salts on the surface of carbon. Their catalytic activity was examined in ammonia borane (NH3BH3) hydrolysis to generate hydrogen gas. This nanomaterial exhibits a higher catalytic activity than those of monometallic and bimetallic counterparts and a stoichiometric amount of hydrogen was produced at a high generation rate. Hydrogen production rates were investigated in different concentrations of NH3BH3 solutions, including in the borates saturated solution, showing little influence of the concentrations on the reaction rates. The hydrogen production rate can reach 3.6-3.8 mol H2 molcat -1 min-1 at room temperature (21 °C). The activation energy and TOF value are 38.36 kJ/mol and 93.8 mol H2 molcat -1 min-1, respectively, comparable to those of Pt based catalysts. This nanomaterial catalyst also exhibits excellent chemical stability, and no significant morphology change was observed from TEM after the reaction. Using this catalyst for continuously hydrogen generation, the hydrogen production rate can be kept after generating 6.2 L hydrogen with over 10,000 turnovers and a TOF value of 90.3 mol H2 molcat -1 min-1.

  14. NiAl{sub 2}O{sub 4} catalysts prepared by combustion reaction using glycine as fuel

    Energy Technology Data Exchange (ETDEWEB)

    Leal, Elvia [Department of Materials Engineering - UFCG, Av. Aprigio Veloso - 882, Bodocongo, 58109-970 Campina Grande, PB (Brazil); Figueiredo de Melo Costa, Ana Cristina, E-mail: anacristina@dema.ufcg.edu.br [Department of Materials Engineering - UFCG, Av. Aprigio Veloso - 882, Bodocongo, 58109-970 Campina Grande, PB (Brazil); Lino de Freita, Normanda; Lucena Lira, Helio de [Department of Materials Engineering - UFCG, Av. Aprigio Veloso - 882, Bodocongo, 58109-970 Campina Grande, PB (Brazil); Goldschmidt Aliaga Kiminami, Ruth Herta [Department of Materials Engineering - UFSC, Rod. Washington Luiz, km 235, 13565-905 Sao Carlos, SP (Brazil); Gama, Lucianna [Department of Materials Engineering - UFCG, Av. Aprigio Veloso - 882, Bodocongo, 58109-970 Campina Grande, PB (Brazil)

    2011-09-15

    Graphical abstract: The reaction temperature was found to remain is practically constant throughout the interval preceding ignition, after which the temperature increased abruptly, reaching the maximum combustion temperature. All the reactions occurred in a matter of minutes, i.e., 5.8, 5.8 and 6 min, respectively, for compositions GES, 10GE and 20GE. Among the benefits of the combustion synthesis method are low processing cost, energy efficiency, high production rate and, especially, short reaction periods when compared with conventional methods (solid state reaction) to prepare ceramic oxide powders that require high calcination temperatures and long reaction periods. Highlights: {yields} We use a simple, fast and inexpensive technique for processing NiAl{sub 2}O{sub 4} catalyst nanopowders. {yields} We study the preparation of powders with nanometric sized particles. {yields} This material is extremely attractive for use in the development of new catalysts for a variety of chemical processes. {yields} Nanometric sized particles depend of the amount of glycine used in the synthesis process. -- Abstract: The aim of this work is to evaluate the influence of glycine fuel used in a stoichiometric proportion and with a 10% and 20% excess of this fuel in the preparation of NiAl{sub 2}O{sub 4} catalyst by combustion reaction. The powders were characterized by XRD, textural analysis by the BET nitrogen adsorption method, particle size distribution, and FTIR. The results show the presence of NiAl{sub 2}O{sub 4} as a major phase and traces of NiO and Ni in all the catalysts studied here. The crystallite sizes were 22 nm in the stoichiometric composition and 18 and 9 nm, respectively, in the composition containing 10% and 20% excess glycine. The powder obtained from all the compositions presented morphological characteristics with irregular plate-shaped agglomerates. The increase in excess glycine caused the particle size in the three compositions to decrease to 59, 54 and

  15. A study concerning the pretreatment of CNTs and its influence on the performance of NiB/CNTs amorphous catalyst

    Directory of Open Access Journals (Sweden)

    CHANG YUAN HU

    2006-11-01

    Full Text Available As prepared carbon nanotubes were pretreated with nitric acid (CNTs-HNO3 or ammonia (CNTs-NH3. Fourier transform infrared spectroscopy (FTIR measurements showed that the surface of the nanotubes was functionalized with carboxylic and hydroxyl functional groups after the acid treatment and that basic groups containing nitrogen, such as N–H and C–N, were introduced to the surface of the nanotubes after the ammonia treatment. X-Ray diffraction analysis implied that the nickel residue in the CNTs was effectively removed by acid treatment. However, the nickel residue was only partially eliminated by ammonia pretreatment. NiB amorphous catalysts supported on CNTs-HNO3 and CNTs-NH3 were prepared by the impregnation–chemical reduction method and characterized by transmission electron microscopy (TEM, as well as inductively coupled plasma (ICP spectroscopy and studied in the selective hydrogenation of acetylene. TEM measurements showed that a high density NiB particles of about 9 nm were homogeneously dispersed on the CNTs-NH3. However, NiB particles (13–23 nmwith amean size of 16 nm were scattered on the CNTs-HNO3. As a result, the activity and selectivity of NiB/CNTs-NH3 were higher than those of NiB/CNTs-HNO3 in the selective hydrogenation of acetylene.

  16. H2 Production over Ni/γ-Al2O3 Catalyst Prepared by a Homogeneous Precipitation Method Using Urea for Direct Internal Reforming (DIR) in a Molten Carbonate Fuel Cell (MCFC)

    National Research Council Canada - National Science Library

    Roh, Hyun-Seog; Jung, Youshick; Koo, Kee Young; Jung, Un Ho; Seo, Yong-Seog; Yoon, Wang Lai

    2009-01-01

    Ni/γ-Al2O3 catalysts (Ni content = 52 wt %) have been designed by a homogeneous precipitation method using urea as a precipitation agent for direct internal reforming in a molten carbonate fuel cell...

  17. The Influence of Promoter on Ni(15)/La(5)/γ-Al2O3 Catalyst in CO2-Steam Reforming of Methane to Syngas at High Pressure.

    Science.gov (United States)

    Ok, Hye Jeong; Park, Myung Hee; Moon, Dong Ju; Kim, Jong Ho; Park, Nam Cook; Kim, Young Chul

    2015-01-01

    Catalysts were investigated with respect to catalytic activity and coke formation in combined steam and carbon dioxide reforming of methane to develop a highly active and stable catalyst for gas to liquid processes. Ni/La-X/Al2O3 (X = Co, Ce, Mo) catalysts were prepared by an impregnation method. The combined steam and carbon dioxide reforming of methane reaction were studied as a function of high pressure (20 bar) in a fixed bed reactor system. X-ray diffraction, BET surface area, and H2-temperature programmed reduction were used to observe the characteristics of the prepared catalysts. Coke formation of used catalysts was examined by scanning electron microscopy, transmission electron microscopy and the coke amount of used catalysts was measured by thermo gravimetric analysis. Catalysts with smaller particle size had a higher temperature of reduction, which had a positive effect on catalytic activity. The improvement in active site rise and dispersion and the lowest metal crystal size had an effect on catalyst activity. As a result, the Ni/La-Co/Al2O3 catalyst showed the highest activity at a reaction temperature of 800 degrees C and a reaction pressure of 20 bar.

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

    Directory of Open Access Journals (Sweden)

    Viviana Ospina

    2015-08-01

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

  19. Catalytic activity and effect of modifiers on Ni-based catalysts for the dry reforming of methane

    Energy Technology Data Exchange (ETDEWEB)

    Barroso-Quiroga, Maria Martha; Castro-Luna, Adolfo Eduardo [Facultad de Ingenieria y Ciencias Economico-Sociales INTEQUI-CONICET-UNSL, Av. 25 de Mayo 384 (5730) Villa Mercedes (S.L.) (Argentina)

    2010-06-15

    Ni catalysts supported on different ceramic oxides (Al{sub 2}O{sub 3}, CeO{sub 2}, La{sub 2}O{sub 3}, ZrO{sub 2}) were prepared by wet impregnation. The catalytic behavior toward hydrogen production through the dry reforming of methane using a fixed-bed reactor was evaluated under certain experimental conditions, and the catalyst supported on ZrO{sub 2} showed the highest stable activity during the period of time studied. The catalyst supported on CeO{sub 2} has a relatively good activity, but shows signs of deactivation after a certain time during the reaction. This catalyst was chosen to be studied after the addition of 0.5 wt% Li and K as activity modifiers. The introduction of the alkaline metals produces a reduction of the catalytic activity but a better stability over the reactant conversion time. The reverse water-gas shift reaction influences the global system of reactions, and as the results indicate, should be considered near equilibrium. (author)

  20. High efficient conversion of furfural to 2-methylfuran over Ni-Cu/Al2O3 catalyst with formic acid as a hydrogen donor

    DEFF Research Database (Denmark)

    Fu, Zhaolin; Wang, Ze; Lin, Weigang

    2017-01-01

    Conversion of furfural to 2-methylfuran over Cu/Al2O3, Ni/Al2O3 and Ni-Cu/Al2O3 catalysts were investigated with formic acid as a hydrogen donor. Ni/Al2O3 showed a high catalytic activity but a moderate selectivity to 2-methylfuran. Contrarily, Cu/Al2O3 showed a low catalytic activity but a high...... selectivity for carbonyl reduction. Over the bimetallic catalysts Ni-10%Cu/Al2O3, by increasing Ni content, more furfural was converted with the reduction of carbonyl primarily. The effect of reaction solvent and the fraction of formic acid were also studied. The result showed that isopropanol solvent could...

  1. Catalytic Steam Reforming of Toluene as a Model Compound of Biomass Gasification Tar Using Ni-CeO2/SBA-15 Catalysts

    Directory of Open Access Journals (Sweden)

    Erik Dahlquist

    2013-07-01

    Full Text Available Nickel supported on SBA-15 doped with CeO2 catalysts (Ni-CeO2/SBA-15 was prepared, and used for steam reforming of toluene which was selected as a model compound of biomass gasification tar. A fixed-bed lab-scale set was designed and employed to evaluate the catalytic performances of the Ni-CeO2/SBA-15 catalysts. Experiments were performed to reveal the effects of several factors on the toluene conversion and product gas composition, including the reaction temperature, steam/carbon (S/C ratio, and CeO2 loading content. Moreover, the catalysts were subjected to analysis of their carbon contents after the steam reforming experiments, as well as to test the catalytic stability over a long experimental period. The results indicated that the Ni-CeO2/SBA-15 catalysts exhibited promising capabilities on the toluene conversion, anti-coke deposition and catalytic stability. The toluene conversion reached as high as 98.9% at steam reforming temperature of 850 °C and S/C ratio of 3 using the Ni-CeO2(3wt%/SBA-15 catalyst. Negligible coke formation was detected on the used catalyst. The gaseous products mainly consisted of H2 and CO, together with a little CO2 and CH4.

  2. Hydrogen production by oxidative reforming of hexadecane over Ni and Pt catalysts supported on Ce/La-doped Al{sub 2}O{sub 3}

    Energy Technology Data Exchange (ETDEWEB)

    Navarro, R.M.; Alvarez-Galvan, M.C.; Fierro, J.L.G. [Instituto de Catalisis y Petroleoquimica (CSIC), C/Marie Curie 2, Cantoblanco 28049, Madrid (Spain); Rosa, F. [Centro de experimentacion de ' El Arenosillo' (CEDEA), Instituto Nacional de Tecnica Aeroespacial (INTA), Ctra. de San Juan del Puerto-Matalascanas km 31, 21130 Mazagon-Moguer (Spain)

    2006-01-04

    The activity and selectivity to hydrogen of alumina-supported nickel or platinum catalysts doped with Ce and La for the oxidative reforming of hexadecane were studied. The influence of both thermal stabilizer and activity promoter, such as lanthanum and cerium oxide, respectively, over hydrogen yield and catalyst durability was investigated. Catalytic activity was found to depend strongly on the type of metal, platinum showing lower specific activities per atom of metal exposed and a higher selectivity to combustion products than the Ni counterparts. The characterization results achieved with H{sub 2} chemisorption, XRD, TPR and XPS showed differences in surface metal concentrations and metal-support interactions which depend on the presence of cerium and/or lanthanum in the support composition. For both based metal catalysts higher reforming activities were found when active metals were deposited on Ce-La-Al{sub 2}O{sub 3} substrate. For Pt-based catalysts, the increase in activity observed for the sample using Ce-La-modified alumina as support is suggested to be related with a participation of lanthanum in the reaction more than modifications on coke resistance or dispersion and state of platinum-induced by lanthanum. In the case of Ni-based catalysts, a lower carbon deposition and a higher thermal stability of metallic Ni particles under reaction conditions were observed for catalyst using Ce-La-modified alumina as support. It is suggested that the higher number of Ni-Ce and Ni-Al surface interactions developed Ce-La-Al{sub 2}O{sub 3}-supported Ni catalysts are responsible of the better catalytic behaviour of this sample in the oxidative reforming of hexadecane.

  3. Hydroconversion of Waste Cooking Oil into Green Biofuel over Hierarchical USY-Supported NiMo Catalyst: A Comparative Study of Desilication and Dealumination

    Directory of Open Access Journals (Sweden)

    Zongwei Zhang

    2017-09-01

    Full Text Available The hydroconversion of waste cooking oil into hydrocarbon fuel was investigated over the hierarchical USY zeolite-supported NiMo catalysts which were prepared by dealumination ((NH42SiF6/desilication (NaOH. The physical and acidity properties of the hierarchical catalysts were characterized by X-ray diffraction (XRD, the Brunauer-Emmett-Teller (BET infrared spectroscopy of adsorbed pyridine (Py-IR, ammonia temperature-programmed desorption (NH3-TPD, and H2 temperature-programmed reduction (H2-TPR. The Brønsted/Lewis (B/L acid distribution was little affected by dealumination and the acid density decreased significantly. However, the highly-desilicated catalysts decreased the B/L ratio obviously. Therefore, many more Mo species in the NiMoO4− and MoO3 phases were produced in the AHFS-treated catalysts, while more high-valence-state Mo species in the NiMoO4− phase were formed in the NaOH-treated catalysts. The AHFS-treated catalysts showed higher catalytic activity and better DCO2 selectivity and selective cracking for jet fuel. The 42.3% selectivity of jet fuel and 13.5% selectivity of jet-range aromatics was achieved over the 8 wt % (NH42SiF6-treated catalyst with 67% DCO2 selectivity.

  4. Microemulsion-prepared Ni catalysts supported on cerium-lanthanum oxide for the selective catalytic oxidation of ammonia in gasified biomass

    Energy Technology Data Exchange (ETDEWEB)

    Nassos, S.; Svensson, E. Elm; Nilsson, M.; Boutonnet, M.; Jaeraas, S. [KTH, Royal Institute of Technology, Chemical Engineering and Technology, Chemical Technology, Teknikringen 42, S-10044 Stockholm (Sweden)

    2006-04-18

    Nickel (Ni) catalysts supported on cerium-lanthanum oxide were prepared by two different preparation techniques and have been tested in the temperature range of 500-750{sup o}C for selective catalytic oxidation of ammonia to nitrogen in gasified biomass. The two different catalyst preparation methods used are the conventional and the microemulsion (water-in-oil). The effect on catalytic activity of different Ni loadings was also tested in combination with the preparation method. Catalyst characterisation was focused on BET and XRD analysis. Cordierite monoliths were used in a tubular quartz reactor for the purpose of the activity tests. For simulating the gasified biomass fuel, 400ppm NH{sub 3} was added to the fuel. Water was also present during the activity tests, which were carried out at fuel rich conditions. Results showed that the microemulsion-prepared catalysts obtained higher performance than the conventional ones, with the best catalyst reaching 98% ammonia conversion and 99% nitrogen selectivity at 750{sup o}C. The more the Ni supported on the catalyst, the higher the catalytic activity. Constant conversion and negligible carbon deposition were two other important characteristics for the microemulsion-prepared catalysts. (author)

  5. Raney copper catalysts for the water-gas shift reaction: I. Preparation, activity and stability

    CSIR Research Space (South Africa)

    Mellor, JR

    1997-12-23

    Full Text Available disper- sion is expressed in terms of the ratio of the total number of surface atoms to the total number of metal atoms present. Copper particle volume-area mean diameter (dvA) was calculated according to the pro- cedure outlined by Anderson et al...

  6. Concentration of ions Co(II), Ni(II) at the Tokem-250 carboxylic cation exchange for catalysts development

    Science.gov (United States)

    Zharkova, Valentina; Bobkova, Ludmila; Brichkov, Anton; Kozik, Vladimir

    2017-11-01

    Sorption and catalytic properties of the cation exchanger are investigated. It was found that the Tokem-250 has a wide operating range of pH. The value of the effective ionization constant of the functional groups of the cation exchanger (pKa) is 6.59. The Tokem-250 cation exchanger exhibits selectivity to Ni2+ ions to Co2+ (D˜103). This is probably due to the stability of ion-exchange complexes detected by the method of diffuse reflectance electron spectroscopy (ESDD). According to these data, for Co2+ ions, in contrast to Ni2+, tetragonal distortion of octahedral coordination is characteristic, which has a positive effect on the stability of complexes with Co2+. To obtain spherical catalysts on the basis of Tokem-250, cobalt-containing samples of cation exchanger were used. The developed spherical materials have catalytic activity in the reactions of deep and partial oxidation of n-heptane.

  7. Ni-M-O (M=Sn, Ti and W) catalysts prepared from dry mixing method for oxidative dehydrogenation of ethane

    KAUST Repository

    Zhu, Haibo

    2016-03-25

    A new generation of Ni-Sn-O, Ni-Ti-O, and Ni-W-O catalysts has been prepared by a solid state grinding method. In each case the doping metal varied from 2.5% to 20%. These catalysts exhibited higher activity and selectivity for ethane oxidative dehydrogenation (ODH) than conventionally prepared mixed oxides. Detailed characterisation was achieved using XRD, N2 adsorption, H2-TPR, SEM, TEM, and HAADF-STEM in order to study the detailed atomic structure and textural properties of the synthesized catalysts. Two kinds of typical structures are found in these mixed oxides, which are (major) “NixMyO” (M = Sn, Ti or W) solid solution phases (NiO crystalline structure with doping atom incorporated in the lattice) and (minor) secondary phases (SnO2, TiO2 or WO3). The secondary phase exists as a thin layer around small “NixMyO” particles, lowering the aggregation of nanoparticles during the synthesis. DFT calculations on the formation energies of M-doped NiO structures (M = Sn, Ti, W) clearly confirm the thermodynamic feasibility of incorporating these doping metals into NiO struture. The incorporation of doping metals into the NiO lattice decreases the number of holes (h+) localized on lattice oxygen (O2- + h+ ➔ O●-), which is the main reason for the improved catalytic performance (O●- is known to favor complete ethane oxidation to CO2). The high efficiency of ethylene production achieved in these particularly prepared mixed oxide catalysts indicates that the solid grinding method could serve as a general and practical approach for the preparation of doped NiO based catalysts.

  8. Screening single-atom catalysts for methane activation: α -A l2O3(0001 ) -supported Ni

    Science.gov (United States)

    Gao, Fei; Gao, Shiwu; Meng, Sheng

    2017-08-01

    Methane activation is one of the biggest challenges for chemical conversion of hydrocarbons and fundamental science. We systematically screen d -block transition metal elements as potential candidates of single-atom catalysts (SACs) for methane dissociation. The adsorption of methane on free metal atoms strongly depends on the number of d electrons of SAC, where the maximum binding energy is formed with the Ni group (electronic configuration d8s2 or d9s1 ). Interestingly, the magnetic moment of the SACs decreases by 2 μB for strong interactions, suggesting that the methane-metal bond forms a spin singlet state involving two electrons of opposite spins. To examine the effect of substrates, the screened transition metals, Ni, Rh, and Pt are further put onto prototype metal oxide surfaces. The substrate dramatically modifies the discrete energy levels of a single metal and its catalytic properties. Single Ni atoms supported on an O-terminated α -A l2O3(0001 ) surface (N i1/A l2O3 ) show superior catalytic properties, with a low activation barrier of 0.4 eV (0.11 eV after zero-point energy correction) for the C-H bond dissociation and simultaneously an extreme stability with a high binding energy of ˜9.39 eV for the Ni anchor. This work identifies N i1/A l2O3 catalyst as an optimal SAC and offers new atomistic insights into the mechanism of methane activation on SACs.

  9. Methane dry reforming over Ni catalysts supported on Ce–Zr oxides prepared by a route involving supercritical fluids

    Directory of Open Access Journals (Sweden)

    Smirnova Marina Yu.

    2017-12-01

    Full Text Available Ce0.5Zr0.5O2 mixed oxides were prepared in a flow reactor in supercritical isopropanol with acetylacetone as a complexing agent. Variation of the nature of the Zr salt and the temperature of synthesis affected the phase composition, morphology and specific surface area of oxides. X-ray diffraction and Raman spectroscopy studies revealed formation of metastable t” and t’ phases. Oxides are comprised of agglomerates with sizes depending on the synthesis parameters. Loading NiO decreases the specific surface area without affecting X-ray particle sizes of supports. Such sintering was the most pronounced for a support with the highest specific surface area, which resulted in the lowest surface content of Ni as estimated by X-ray photoelectron spectroscopy and in the formation of flattened NiO particles partially embedded into the support. The catalytic activity and stability of these samples in the dry reforming of methane were determined by the surface concentration of Ni and the morphology of its particle controlled by the metal-support interaction, which also depends on the type of catalyst pretreatment. Samples based on ceria-zirconia oxides prepared under these conditions provide a higher specific catalytic activity as compared with the traditional Pechini route, which makes them promising for the practical application.

  10. Enhancement of Glycerol Steam Reforming Activity and Thermal Stability by Incorporating CeO2 and TiO2 in Ni- and Co-MCM-41 Catalysts

    Science.gov (United States)

    Dade, William N.

    Hydrogen (H2) has many applications in industry with current focus shifted to production of hydrocarbon fuels and valuable oxygenates using the Fischer-Tropsch technology and direct use in proton exchange membrane fuel cell (PEMFC). Hydrogen is generally produced via steam reforming of natural gas or alcohols like methanol and ethanol. Glycerol, a by-product of biodiesel production process, is currently considered to be one of the most attractive sources of sustainable H2 due to its high H/C ratio and bio-based origin. Ni and Co based catalysts have been reported to be active in glycerol steam reforming (GSR); however, deactivation of the catalysts by carbon deposition and sintering under GSR operating conditions is a major challenge. In this study, a series of catalysts containing Ni and Co nanoparticles incorporated in CeO2 and TiO2 modified high surface area MCM-41 have been synthesized using one-pot method. The catalysts are tested for GSR (at H2O/Glycerol mole ratio of 12 and GHSV of 2200 h-1) to study the effect of support modification and reaction temperature (450 - 700 °C) on the product selectivity and long term stability. GSR results revealed that all the catalysts performed significantly well exhibiting over 85% glycerol conversion at 650 °C except Ni catalysts that showed better low temperature activities. Deactivation studies of the catalysts conducted at 650 °C indicated that the Ni-TiO2-MCM-41 and Ni-CeO 2-MCM-41 were resistant to deactivation with ˜100% glycerol conversion for 40 h. In contrast, Co-TiO2-MCM-41 perform poorly as the catalyst rapidly deactivated after 12 h to yield ˜20% glycerol conversion after 40 h. The WAXRD and TGA-DSC analyses of spent catalysts showed a significant amount of coke deposition that might explain catalysts deactivation. The flattening shape of the original BET type IV isotherm with drastic reduction of catalyst surface area can also be responsible for observed drop in catalysts activities.

  11. Well-dispersed Ni nanoclusters on the surfaces of MFI nanosheets as highly efficient and selective catalyst for the hydrogenation of naphthalene to tetralin

    Science.gov (United States)

    Gong, Pengyu; Li, Baoshan; Kong, Xianglong; Liu, Jianjun; Zuo, Shengli

    2017-11-01

    One of the challenges in material science has been to design and prepare highly efficient and selective catalysts for target reactions. Here we demonstrate a one-pot hydrothermal synthesis of hierarchical MFI nanosheets with nickel species chemically bonded on the outer surfaces. It turns out that the growth and morphologies of self-pillared MFI nanosheets are affected by Ni content, and the thickness of MFI nanosheets are determined to be 2.3 nm or 3.0 nm. Specially, the bonded Ni on the outer surfaces can effectively prevent adjacent nanosheets from forming new Sisbnd Osbnd Si bonds, and in conjunction with the self-pillared structure, can hamper complete collapse of Ni-MFI-NSs during calcination. In naphthalene hydrogenation, the separated Ni species are previously reduced to highly-dispersed metallic Ni nanoclusters with size below 1.6 nm, which are highly active for hydrogenation. And the hierarchical porosity of Ni-MFI-NSs significantly enhances the diffusion of substrates and the accessibility of active sites. As a result, Ni-MFI-NSs achieve 100% selectivity for tetralin and 84.9% conversion of naphthalene with Ni content of only 4.2 wt%. Furthermore, the gradually enlarged Ni nanoparticles cause the decline of catalytic activities of catalysts.

  12. Syngas Production from Catalytic CO2 Reforming of CH4 over CaFe2O4 Supported Ni and Co Catalysts: Full Factorial Design Screening

    Directory of Open Access Journals (Sweden)

    M. Anwar Hossain

    2018-01-01

    Full Text Available In this study, the potential of dry reforming reaction over CaFe2O4 supported Ni and Co catalysts were investigated. The Co/CaFe2O4 and Ni/CaFe2O4 catalysts were synthesized using wet impregnation method by varying the metal loading from 5-15 %. The synthesized catalysts were tested in methane dry reforming reaction at atmospheric pressure and reaction temperature ranged 700-800 oC. The catalytic performance of the catalysts based on the initial screening is ranked as 5%Co/CaFe2O4 < 10%Co/CaFe2O4 < 5%Ni/CaFe2O4 < 10%Ni/CaFe2O4 according to their performance. The Ni/CaFe2O4 catalyst was selected for further investigation using full factorial design of experiment. The interaction effects of three factors namely metal loading (5-15 %, feed ratio (0.4-1.0, and reaction temperature (700-800 oC were evaluated on the catalytic activity in terms of CH4 and CO2 conversion as well as H2 and CO yield. The interaction between the factors showed significant effects on the catalyst performance at metal loading, feed ratio and reaction temperature of 15 %, 1.0, and 800 oC. respectively. The 15 wt% Ni/CaFe2O4 was subsequently characterized by Thermogravimetric (TGA, X-ray Diffraction (XRD, Field Emission Scanning Electron Microscopy (FESEM, Energy Dispersive X-ray Spectroscopy (EDX, X-ray Photoelectron Spectroscopy (XPS, N2-physisorption, Temperature Programmed Desorption (TPD-NH3, TPD-CO2, and Fourier Transform Infra Red (FTIR to ascertain its physiochemical properties.  This study demonstrated that the CaFe2O4 supported Ni catalyst has a good potential to be used for syngas production via methane dry reforming. Copyright © 2018 BCREC Group. All rights reserved Received: 5th May 2017; Revised: 8th August 2017; Accepted: 9th August 2017; Available online: 22nd January 2018; Published regularly: 2nd April 2018 How to Cite: Hossain, M.A., Ayodele, B.V., Cheng, C.K., Khan, M.R. (2018. Syngas Production from Catalytic CO2 Reforming of CH4 over CaFe2O4 Supported

  13. Recovery of nickel from spent NiO/Al2O3 catalyst through sulfuric acid leaching, precipitation and solvent extraction.

    Science.gov (United States)

    Nazemi, M K; Rashchi, F

    2012-05-01

    Effective recovery of nickel (Ni) from spent NiO/Al(2)O(3) catalyst in a simple hydrometallurgical route is suggested. Nickel recovery of 99.5% was achieved with sulfuric acid leaching. The leach liquor was partly neutralized and nickel ammonium sulfate was precipitated by adding ammonia. The nickel in the supernatant was concentrated by solvent extraction using D2EHPA and subsequently stripped back into sulfuric acid and returned to the precipitation stage. Necessary counter current extraction and stripping stages were determined in McCabe-Thiele diagrams. The suggested method appears simple and very effective in recovering nickel from spent catalysts from the petrochemical industry.

  14. Performance of Ni/dolomite pellet catalyst on gas distribution from cassava rhizome gasification with a modular fixed-bed gasifier.

    Science.gov (United States)

    Sricharoenchaikul, V; Atong, D; Sornkade, P; Nisamaneenate, J

    2017-05-01

    Thermal conversion of cassava rhizome was performed using a modular downdraft gasifier with the addition of Ni-based catalysts as promising tar eliminating and produced gas upgrading techniques. The activities of a synthesized 5% Ni/dolomite pellet catalyst prepared by impregnation method were investigated in a secondary reactor downstream of the gasifier. High reforming activity of the Ni/dolomite pellet catalyst on tar reduction was achieved. The conversion to H 2 and CO was improved via steam reforming of methane and char reaction with CO 2 . Moreover, the formation of CH 4 and C x H y was diminished through the tar or condensable hydrocarbon reformed on the catalyst surface. The carbon and hydrogen conversions of cassava rhizome with prepared catalyst were 83.79% and 61.78%, respectively, at an air flow rate of 1.98 m 3 /hr. At this condition, tar formation was low, while the lower heating value was 4.39 MJ/m 3 and H 2 to CO molar ratio was 1.22. Generally, the addition of a catalyst not only enhanced gas production, but also reduced tar and particulate matter generation; thus, its implementation should help lessen the pollution control requirement and cost of operation, while allowing higher quality fuel gas production.

  15. Catalytic dehydrofluorination of 1,1,1,3,3-pentafluoropropane to 1,3,3,3-tetrafluoropropene over fluorinated NiO/Cr2O3 catalysts

    Science.gov (United States)

    Luo, Jian-Wei; Song, Jian-Dong; Jia, Wen-Zhi; Pu, Zhi-Ying; Lu, Ji-Qing; Luo, Meng-Fei

    2018-03-01

    Catalytic dehydrofluorination of 1,1,1,3,3-pentafluoropropane to 1,3,3,3-tetrafluoropropene was performed on a series of fluorinated NiO/Cr2O3 catalysts. The NiO/Cr2O3 catalysts were more active than the Cr2O3 because the new acid sites provided by NiF2 had higher turnover frequencies (9.43 × 10-3 - 12.08 × 10-3 s-1) than those on the Cr2O3 (4.55 × 10-3 s-1). Also, the NiO/Cr2O3 was more stable than the Cr2O3 due to its lower density of surface acid sites, which alleviated the coke deposition on the catalyst as evidenced by the Raman spectroscopic results. The kinetic results revealed that the15NiO/Cr2O3 had much lower activation energy (63.6 ± 4.5 kJ mol-1) than the Cr2O3 (127.6 ± 3.8 kJ mol-1). Accordingly, different reaction pathways on the two catalysts were proposed, which involved the cleavage of the Csbnd F and Csbnd H bonds on the surface acid and base sites, respectively.

  16. Low-Temperature Catalytic Performance of Ni-Cu/Al2O3 Catalysts for Gasoline Reforming to Produce Hydrogen Applied in Spark Ignition Engines

    Directory of Open Access Journals (Sweden)

    Le Anh Tuan

    2016-03-01

    Full Text Available The performance of Ni-Cu/Al2O3 catalysts for steam reforming (SR of gasoline to produce a hydrogen-rich gas mixture applied in a spark ignition (SI engine was investigated at relatively low temperature. The structural and morphological features and catalysis activity were observed by X-ray diffractometry (XRD, scanning electron microscopy (SEM, and temperature programmed reduction (TPR. The results showed that the addition of copper improved the dispersion of nickel and therefore facilitated the reduction of Ni at low temperature. The highest hydrogen selectivity of 70.6% is observed over the Ni-Cu/Al2O3 catalysts at a steam/carbon ratio of 0.9. With Cu promotion, a gasoline conversion of 42.6% can be achieved at 550 °C, while with both Mo and Ce promotion, the gasoline conversions were 31.7% and 28.3%, respectively, higher than with the conventional Ni catalyst. On the other hand, initial durability testing showed that the conversion of gasoline over Ni-Cu/Al2O3 catalysts slightly decreased after 30 h reaction time.

  17. Fabrication of vertical GaN/InGaN heterostructure nanowires using Ni-Au bi-metal catalysts.

    Science.gov (United States)

    Ha, Ryong; Kim, Sung-Wook; Choi, Heon-Jin

    2013-06-26

    We have fabricated the vertically aligned coaxial or longitudinal heterostructure GaN/InGaN nanowires. The GaN nanowires are first vertically grown by vapor-liquid-solid mechanism using Au/Ni bi-metal catalysts. The GaN nanowires are single crystal grown in the [0001] direction, with a length and diameter of 1 to 10 μm and 100 nm, respectively. The vertical GaN/InGaN coaxial heterostructure nanowires (COHN) are then fabricated by the subsequent deposition of 2 nm of InxGa1-xN shell on the surface of GaN nanowires. The vertical GaN/InGaN longitudinal heterostructure nanowires (LOHN) are also fabricated by subsequent growth of an InGaN layer on the vertically aligned GaN nanowires using the catalyst. The photoluminescence from the COHN and LOHN indicates that the optical properties of GaN nanowires can be tuned by the formation of a coaxial or longitudinal InGaN layer. Our study demonstrates that the bi-metal catalysts are useful for growing vertical as well as heterostructure GaN nanowires. These vertically aligned GaN/InGaN heterostructure nanowires may be useful for the development of high-performance optoelectronic devices.

  18. CH4-CO2 reforming in surface DBD reactor with ZnO-Cu and NiO catalysts

    Science.gov (United States)

    Lazzaroni, Claudia; Rahmani, Abdelkader; Nikravech, Mehrdad; MP4 Team

    2015-09-01

    Dry reforming of methane (CH4) is carried out in an atmospheric pressure Dielectric Barrier Discharge (DBD) reactor. The two 3 mm thickness aluminum electrodes are separated by a 3 mm thickness dielectric sheet made of quartz. The electrodes present 3 branches and the space between two adjacent branches is filled with beads of catalyst which are 2 mm diameter alumina beads coated with ZnO-Cu or NiO. The coating is performed in two different ways: (i) by impregnation and (ii) by fluidized spray plasma. A 30 kHz and several kV AC voltage is applied to the electrodes. The feedstock gas is a mixture of argon, carbon dioxide (CO2) and methane with individual fluxes varying from 20 to 80 mL/min. At the reactor outlet, the gas goes through a condenser at 4°C to condense liquid products. The reforming reaction products are identified by liquid and gas phase chromatography. The effect of the applied power and the catalyst nature on the product distribution is studied. Whatever the catalyst, the conversion rate of CH4 and CO2 increases with the applied power while the selectivity of gas products is almost independent of the power. The condensed liquids collected under our experimental conditions, such as ethanol or acetic acid, represent more than 10% of the products. This work is partially supported by the Programme Interdisciplinaire SPC: Énergie, Société, Territoire.

  19. A potentially implantable glucose fuel cell with Raney-platinum film electrodes for improved hydrolytic and oxidative stability

    Energy Technology Data Exchange (ETDEWEB)

    Kerzenmacher, S.; Kraeling, U.; Metz, T.; von Stetten, F. [Laboratory for MEMS Applications, Department of Microsystems Engineering - IMTEK, University of Freiburg, Georges-Koehler-Allee 103, D-79110 Freiburg (Germany); Zengerle, R. [Laboratory for MEMS Applications, Department of Microsystems Engineering - IMTEK, University of Freiburg, Georges-Koehler-Allee 103, D-79110 Freiburg (Germany); Centre for Biological Signalling Studies (bioss), Albert-Ludwigs-Universitaet Freiburg (Germany)

    2011-02-01

    We present an improved abiotically catalyzed glucose fuel cell, intended as energy harvesting tissue implantable power supply for medical implants. The fuel cell is constructed from a Raney-platinum film cathode deposited on a silicon substrate with micro-machined feedholes for glucose permeability, arranged in front of a Raney-platinum film anode. A novelty is the application of platinum for both electrodes and the complete abdication of hydrogel binders. This overcomes the limited stability against hydrolytic and oxidative attack encountered with previous glucose fuel cells fabricated from activated carbon particles dispersed in a hydrogel matrix. During performance characterization in phosphate buffered saline under physiological concentrations of glucose and oxygen the diffusion resistance to be expected from tissue capsule formation was taken into account. Despite the resulting limited oxygen supply, the Raney-platinum fuel cells exhibit a power density of up to (4.4 {+-} 0.2) {mu}W cm{sup -2} at 7.0% oxygen saturation. This exceeds the performance of our previous carbon-based prototypes, and can be attributed to the higher catalytic activity of platinum cathodes and in particular the increased oxygen tolerance of the Raney-platinum film anodes. (author)

  20. Immobilization of a layer of carbon nanofibres (CNFs) on Ni foam: A new structured catalyst support.

    NARCIS (Netherlands)

    Jarah nabeel abdul kareem amin, N.A.K.A.; Jarrah, Nabeel A.; Li, F.; van Ommen, J.G.; Lefferts, Leonardus

    2005-01-01

    This work describes the preparation of new materials based on immobilizing carbon nanofibres (CNFs) on the surface of Ni foam. CNFs were catalytically synthesized by decomposition of ethene over the Ni foam. The influence of formation conditions on the morphology of the CNFs, on the mechanical

  1. Effects of pH and chelating agent on the NiWS phase formation in NiW/γ-Al{sub 2}O{sub 3} HDS catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Santolalla-Vargas, C.E.; Suárez Toriello, V.A. [Universidad A. Metropolitana-Iztapalapa, Área de Ingeniería Química, Av. FFCC R, Atlixco 186, Vicentina, 09340 Distrito Federal (Mexico); Reyes, J.A. dos, E-mail: jarh@xanum.uam.mx [Universidad A. Metropolitana-Iztapalapa, Área de Ingeniería Química, Av. FFCC R, Atlixco 186, Vicentina, 09340 Distrito Federal (Mexico); Cromwell, D.K. [University of New Hampshire, Department of Chemical Engineering, 207 Thompson Hall, Durham, NH 03824 (United States); Pawelec, B.; Fierro, J.L.G. [Instituto de Catálisis y Petroleoquímica, CSIC, Cantoblanco, E-28049, Madrid (Spain)

    2015-09-15

    In this article, NiW/γ-Al{sub 2}O{sub 3} samples were prepared by consecutive impregnations of a W/γ-Al{sub 2}O{sub 3}-based catalyst with aqueous solution of nickel salt. The structural control of the nickel ion precursor in the impregnation solution was achieved by the addition of 1,2-cyclohexanediamine-N,N,N′,N′-tetraacetic acid (CyDTA) as a chelating agent. The influence of pH of this aqueous solution on the NiWS phase formation in the sulfided catalysts was investigated. Coordination structures of the Ni–CyDTA complexes were evaluated by FT-IR and DRS UV–Vis spectroscopies. Sulfided catalysts were characterized by X-ray photoelectron spectroscopy (XPS) and high resolution transmission electron microscopy (HRTEM) and tested in hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene (4,6-DMDBT) carried out in a batch reactor at 593 K and total H{sub 2} pressure of 55 bar. Spectroscopic characterization by DRS UV–Vis showed the predominance of the [Ni(CyDTA)]{sup 2−} species in solution. Following the impregnation and drying steps, the [Ni(CyDTA)]{sup 2−} complex showed no apparent changes of its structure, independent of the pH value of impregnation solution. The Ni/W/γ-Al{sub 2}O{sub 3} catalysts ex [Ni(CyDTA)]{sup 2−} complex exhibited high stability. The presence of CyDTA delayed the reduction of Ni and caused a remarkable decrease of the W-support interaction, thus increasing the formation of NiWS phase upon catalyst sulfiding. The catalyst activity–structure correlation demonstrated that the catalyst activity and selectivity is linked with formation of the most active NiWS phase having single or double WS{sub 2} slab structures. The catalyst prepared with [Ni(CyDTA)]{sup 2−} complex at pH of 4.0 exhibited the largest initial HDS activity, which was approximately triple compared with the CyDTA-free counterpart. For all catalysts, the HDS reaction proceeded via hydrogenation (HYD) and direct desulfurization (DDS) reaction routes

  2. Characterization of the various catalyst for solvent hydrogenation at 1t/d PSU; 1t/d PSU ni okeru kakushu yozai suisoka shokubai no seino hyoka

    Energy Technology Data Exchange (ETDEWEB)

    Kakebayashi, H.; Nogami, Y.; Inokuchi, K. [Mitsui SRC Development Co. Ltd., Tokyo (Japan); Aihara, Y.; Imada, K. [Nippon Steel Corp., Tokyo (Japan)

    1996-10-28

    Performance of various catalysts for hydrogenation of recycle solvent was evaluated for the operation of NEDOL process 1 t/d process supporting unit (PSU). Distillate between 220 and 538{degree}C derived from the liquefaction of Tanito Harum coal was used as recycle solvent. Deactivation behaviors of catalysts were compared using a prediction equation of catalyst life, by which aromatic carbon index (fa) after hydrogenation can be determined from the fa of recycle oil before hydrogenation, reaction temperature, and total hydrogenation time. Total hydrogenation time satisfying the {Delta}fa, 0.05 before and after hydrogenation were 8,000, 4,000, and 2,000 hours for NiMo-based catalysts C, A, and B, respectively. Catalyst C showed the longest life. Used catalysts were also characterized. The catalyst C showed larger mean pore size than those of the others, which resulted in the longer life due to the delay of pore blockage. From measurements by XPS and EPMA, relative atomic concentration of carbon increased remarkably after the use for all of catalysts, which was considered to be due to the adhesion of hydrocarbons. Increase of metal atoms, such as Fe and Cr, was also observed due to the contamination of entrainment residues. Deactivation of catalysts was caused by the adhesion of hydrocarbons, and metallic compounds, such as Fe and Cr. 3 refs., 1 fig., 5 tabs.

  3. A structure-activity study of Ni-catalyzed alkyl-alkyl Kumada coupling. Improved catalysts for coupling of secondary alkyl halides.

    Science.gov (United States)

    Ren, Peng; Vechorkin, Oleg; von Allmen, Kim; Scopelliti, Rosario; Hu, Xile

    2011-05-11

    A structure-activity study was carried out for Ni catalyzed alkyl-alkyl Kumada-type cross coupling reactions. A series of new nickel(II) complexes including those with tridentate pincer bis(amino)amide ligands ((R)N(2)N) and those with bidentate mixed amino-amide ligands ((R)NN) were synthesized and structurally characterized. The coordination geometries of these complexes range from square planar, tetrahedral, to square pyramidal. The complexes had been examined as precatalysts for cross coupling of nonactivated alkyl halides, particularly secondary alkyl iodides, with alkyl Grignard reagents. Comparison was made to the results obtained with the previously reported Ni pincer complex [((Me)N(2)N)NiCl]. A transmetalation site in the precatalysts is necessary for the catalysis. The coordination geometries and spin-states of the precatalysts have a small or no influence. The work led to the discovery of several well-defined Ni catalysts that are significantly more active and efficient than the pincer complex [((Me)N(2)N)NiCl] for the coupling of secondary alkyl halides. The best two catalysts are [((H)NN)Ni(PPh(3))Cl] and [((H)NN)Ni(2,4-lutidine)Cl]. The improved activity and efficiency was attributed to the fact that phosphine and lutidine ligands in these complexes can dissociate from the Ni center during catalysis. The activation of alkyl halides was shown to proceed via a radical mechanism. © 2011 American Chemical Society

  4. First-principles study on the Ni@Pt12 Ih core-shell nanoparticles: A good catalyst for oxygen reduction reaction

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Zongxian, E-mail: yzx@henannu.edu.cn [College of Physics and Information Engineering, Henan Normal University, Xinxiang, Henan, 453007 (China); Henan Key Laboratory of Photovoltaic Materials, Xinxiang, 453007 (China); Zhang, Yanxing; Wang, Jinlong; Ma, Shuhong [College of Physics and Information Engineering, Henan Normal University, Xinxiang, Henan, 453007 (China)

    2011-08-15

    The adsorption, diffusion and dissociation properties of O{sub 2} on the icosahedron (Ih) Ni@Pt12 core-shell nanoparticle were investigated using the ab initio density functional theory calculations. It is found that, compared with the Pt(111) surface, the Ih Ni@Pt12 core-shell nanoparticle can enhance the adsorption, diffusion and dissociation of O{sub 2}, as well as the adsorption and diffusion of the atomic O (the dissociation product of O{sub 2}), and therefore serve as a good catalyst for oxygen reduction reaction. Our study gives a reasonable theoretical explanation to the high catalytic activity of the Ni@Pt core-shell nanoparticles for the oxygen reduction reaction. -- Highlights: → The Ni core can enhance the stability of the Ih Ni@Pt12 core-shell nanoparticle. → O{sub 2} prefers the top-bridge-top configuration on the Ih Ni@Pt12. → The Ih Ni@Pt12 can enhance the adsorption, diffusion and the dissociation of O{sub 2}. → The Ih Ni@Pt12 can serve as a good catalyst for the oxygen reduction reaction.

  5. One-Pot 2-Methyltetrahydrofuran Production from Levulinic Acid in Green Solvents Using Ni-Cu/Al2 O3 Catalysts.

    Science.gov (United States)

    Obregón, Iker; Gandarias, Iñaki; Miletić, Nemanja; Ocio, Ainhoa; Arias, Pedro L

    2015-10-26

    The one-pot hydrogenation of levulinic acid to 2-methyltetrahydrofuran (MTHF) was performed using a series of Ni-Cu/Al2 O3 catalysts in green solvents, such as water and biomass-derived alcohols. Ni/Al2 O3 provided the highest activity, whereas Cu/Al2 O3 was the most selective, reaching a 75 % MTHF yield at 250 °C after 24 h reaction time. Synergetic effects were observed when bimetallic Ni-Cu/Al2 O3 catalysts were used, reaching a 56 % MTHF yield in 5 h at 250 °C for the optimum Ni/Cu ratio. Remarkably, these high yields were obtained using non-noble metal-based catalysts and 2-propanol as the solvent. The catalytic activity and selectivity results are correlated to temperature programmed reduction (TPR), XRD, and STEM characterization data, identifying the role associated with mixed Ni-Cu particles in addition to monometallic Cu and Ni. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  6. Effect of a Swelling Agent on the Performance of Ni/Porous Silica Catalyst for CH4-CO2 Reforming.

    Science.gov (United States)

    Amin, Mohamad Hassan; Sudarsanam, Putla; Field, Matthew R; Patel, Jim; Bhargava, Suresh K

    2017-10-10

    Hierarchical porous materials are of great interest in various industrial applications because of their potential to overcome the mass transport limitations typically encountered for single-mode porous materials. This report describes the synthesis of a hierarchical trimodal porous silica-based material using a 7.5 molar ratio of a relatively inexpensive nonionic surfactant template, triblock copolymer P123, EO20PO70EO20. The pore size distribution curve shows the presence of three types of pores with average diameters of ∼8, 25, and 89 nm. Electron microscope images confirm the existence of smaller ordered mesopores (first mode), larger ordered mesopores (second mode), and macropores (third mode). Ni nanoparticles dispersed on this trimodal porous silica produce a material that exhibited excellent catalytic performance for the CO2 reforming of CH4. This research provides new insights that will facilitate the development of trimodal porous silica (TMS) materials for a variety of applications. The results demonstrated that the presence of large pores (second and third mode pores) in TMS material increased the number of accessible active Ni sites, which led to the high activity observed for Ni/TMS catalyst.

  7. Electronic Structure and Reactivity of TM-Doped La1-xSrxCoO3 (TM = Ni, Fe) Catalysts

    Science.gov (United States)

    Grice, S. C.; Flavell, W. R.; Thomas, A. G.; Warren, S.; Marr, P. G.; Jewitt, D. E.; Khan, N.; Dunwoody, P. M.; Jones, S. A.

    The catalytic properties of LaCoO3 in the oxidation of organic molecules in aqueous solution are explored as a function of doping with both Sr substitution for La and Fe and Ni substitution for Co. VUV photoemission is used to explore the surface reactivity of the ceramic catalysts in aqueous solution, using H2O as a probe molecule. These measurements are complemented by EXAFS and XANES measurements designed to probe the local defect structure and by GC measurements of catalytic activity in the aqueous epoxidation of crotyl alcohol. We relate the observed catalytic activity to the defect structure of the doped materials. In Ni-doped materials, oxygen vacancies appear to be the predominant defect, whereas in Fe-doped samples, electron holes are stabilised on Fe, leading to very different behaviour in oxidation. The surface reactivity to water is also influenced by the TM d electron count, with water binding more strongly to Fe-doped materials than to those containing Ni. The influence of these factors on the rate of the unwanted hydrogen peroxide decomposition reaction and hence on activity in epoxidation is discussed.

  8. Direct ethanol fuel cell, CO and ethanol oxidation on core-shell C/Ni-Au-[Pt and (Pt- Ir)] catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Rodrigues, C.A.D.; Tremiliosi-Filho, G. [Universidade de Sao Paulo (IQSC/USP), Sao Carlos, SP (Brazil). Inst. de Quimica], Email: cesaraug@sc.usp.br; Kokoh, K.B.; Coutanceau, C.; Baranton, S. [Universite de Poitiers (France). Lab. de Catalyse en Chimie Organique (LACCO). Equipe Electrocatalyse

    2010-07-01

    In this paper presents to study of the Pt and Pt-Ir monolayer that were deposited on core-shell Ni-Au nanoparticles supported on carbon. Catalysts with the following molar ratios were prepared: Pt and Pt{sub 65}Ir{sub 35}, Pt{sub 75}Ir{sub 2}5, Pt{sub 80}Ir{sub 20} and Pt{sub 85}Ir{sub 15}. The means particle sizes were in the range of 2 - 6 nm for all catalysts. The electrochemical properties examined in the ethanol and CO oxidation by cyclic voltammetry, and In situ IR spectroscopy measurements (SPAIRS) enabled to determine intermediates and reaction products as a function of the metallic compositions of catalysts. All of the catalysts were tested as anodes of a single direct ethanol fuel cell (DEFC) tests in 1.0 M ethanol solution. As a result, higher power densities were obtained with the core-shell particles in comparison to those issued from the commercial catalyst (Pt-ETEK). Thus, the maximum power densities at 90 deg C for the different systems are: (i) commercial C/Pt catalyst (E-TEK): ca. 0.010 W cm{sup -2}, C/Ni-Au-(Pt{sub 85}Ir{sub 15}): ca. 0.013 W cm{sup -2} and C/Ni-Au-Pt: ca. 0.018 W cm{sup -2} (all core-shell systems were normalization by Pt load). As a result, the performance of the core-shell nanoparticles is much better than that produced for the commercial catalyst and the C/Ni-Au-Pt system showed the best performance. (author)

  9. Hydrocracking catalyst made of NiMo sulfide loaded on a modified HEMT zeolite; Catalyseur d`hydrocraquage a base de sulfure de NiMo depose sur une zeolithe HEMT modifiee

    Energy Technology Data Exchange (ETDEWEB)

    Baalala, M.; Bensitel, M. [Universite Chouaib Doukkali, El Jadida (Morocco). Laboratoire de Chimie Physique; Becue, T.; Manoli, J.M. [Universite Pierre et Marie Curie, UMR 7609 CNRS, 75 - Paris (France). Laboratoire Reactivite de Surface; Leglise, J.; Gestel, J.N.M.V.; Lamotte, J.; Goupil, J.M.; Cornet, D. [Caen Univ., UMR 6506 CNRS, ISMRA,14 (France). Laboratoire Catalyse et Spectrochimie

    1999-02-01

    Treating a NH{sub 4}EMT zeolite with a solution of (NH{sub 4}){sub 2}SiF{sub 6} at 80 deg. C affords a solid containing amorphous SiO{sub 2} intimately mixed the zeolite. This acidic support EMT-Si was loaded with NiMo sulfide in order to prepare a bifunctional catalyst, which was tested for the hydrogenation of benzene and the hydrocracking of n-heptane. This NiMo/EMT-Si catalyst was found more active for hydrogenation than the analogous NiMo/HY. This is ascribed to a higher dispersion of the NiMo sulfide, which is almost equally shared between the internal meso-pores in the modified EMT solid, and the fissures, which were created throughout the zeolite grains upon inserting the NiMo sulfide. The catalyst with the EMT-Si support was also found more active than the NiMo/HY for the hydrocracking of heptane, with a slightly higher selectively into heptane isomers. (authors) 14 refs.

  10. Dolomite-Derived Ni-Based Catalysts with Fe Modification for Hydrogen Production via Auto-Thermal Reforming of Acetic Acid

    Directory of Open Access Journals (Sweden)

    Xinyan Zhong

    2016-06-01

    Full Text Available Bio-oil can be obtained via fast pyrolysis of biomass, and typically contains acetic acid (~30 mass %. The acetic acid has often been tested as a model compound for hydrogen production via reforming bio-oil, in which catalysts are a key factor for stable hydrogen production. However, deactivation of catalysts by coking and oxidation hinders the application of the reforming process. Dolomite-derived Ni-based catalysts with Fe additive, MgNi0.2Ca0.8−xFexO2±δ (x = 0–0.8, were successfully synthesized by the hydrothermal synthesis method, and then tested in auto-thermal reforming (ATR of acetic acid (AC. The MgNi0.2Ca0.5Fe0.3O2±δ catalyst performed a stable reactivity in ATR: the conversion of AC reached 100%, and the H2 yield remained stable around 2.6 mol-H2/mol-AC. The catalysts were characterized by X-ray diffraction (XRD, N2 physisorption, X-ray photoelectron spectra (XPS, H2-temperature-programmed reduction (TPR, inductively coupled plasma- atomic emission spectroscopy (ICP-AES and Thermogravimetry (TG; the results show that a periclase-like solid solution of Mg(Ni,FeO and lime were formed via the precursors of dolomite and hydrotalcite, and then transformed into Fe-rich Ni-Fe alloy with basic support of MgO-CaO after reduction. The stable Ni0 spices with basic support can explain the stability and resistance to coking during ATR of AC.

  11. Nitrogen-doped graphene/CoNi alloy encased within bamboo-like carbon nanotube hybrids as cathode catalysts in microbial fuel cells

    Science.gov (United States)

    Hou, Yang; Yuan, Heyang; Wen, Zhenhai; Cui, Shumao; Guo, Xiaoru; He, Zhen; Chen, Junhong

    2016-03-01

    Cost-effective catalysts are of key importance to the successful deployment of microbial fuel cells (MFCs) for electricity generation from organic wastes. Herein, a novel catalyst prepared by one-step synthesis strategy is reported. The catalyst features N-doped bamboo-like carbon nanotube (BCNT) in which CoNi-alloy is encapsulated at the end and/or the middle section of the tube with many graphene layers inside inner cavities of BCNT (N-G@CoNi/BCNT). The prepared N-G@CoNi/BCNT exhibits a high oxygen reduction reaction (ORR) activity with an early onset potential of 0.06 V vs. Ag/AgCl and a comparable exchange current density to that of commercial Pt/C. The excellent catalytic activity is further evidenced by a high electron transfer number of 3.63. When being applied in MFCs, the N-G@CoNi/BCNT yields an average current density of 6.7 A m-2, slightly lower than that of Pt/C but with a less mass transfer potential loss. The cost of the N-G@CoNi/BCNT for constructing a 1-m2 cathode electrode is 200 times lower than that of Pt/C. With such a competitive price and excellent electrocatalytic-activity resulting from its unique morphology, CoNi-alloy/nitrogen dopants, considerable specific surface area, and carbon-coated alloy/graphene hybridization, the present catalyst is a promising candidate for ORR catalysts in MFCs for energy recovery from wastes.

  12. Catalytic decomposition of CH{sub 4} over NiO-Al{sub 2}O{sub 3}-SiO{sub 2} catalysts: Influence of catalyst preparation conditions on the production of H{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Ashok, Jangam; Raju, Gangadhara; Reddy, Padigapati Shiva; Subrahmanyam, Machiraju; Venugopal, Akula [Catalysis and Physical Chemistry Division, Indian Institute of Chemical Technology, Tarnaka, Hyderabad, Andra Pradesh 500 607 (India)

    2008-09-15

    This paper presents the synthesis and characterization of NiO-Al{sub 2}O{sub 3}-SiO{sub 2} catalysts prepared by co-precipitation method and the catalytic activities estimated for the production of H{sub 2} by CH{sub 4} decomposition. The physico-chemical characteristics are evaluated by XRD analysis, TPR and O{sub 2} pulse chemisorption, XPS, CHNS, SEM/EDAX, TEM and BET-surface areas of fresh and used forms of catalysts. XRD studies revealed the presence of hydrotalcite-like precursors in oven dried form and produced dispersed NiO species upon calcination in static air at 450 C. The catalyst compositions for NiO-Al{sub 2}O{sub 3}-SiO{sub 2} system are optimized based on various parameters such as varying Ni loadings, change in Al/Si ratios, precipitation at different pH and finally choice of precursors on CH{sub 4} decomposition activities. Based on the results it is concluded that the composition of NiO-Al{sub 2}O{sub 3}-SiO{sub 2} and preparation conditions played a key role in the decomposition of CH{sub 4}. The optimized compositions are established for the production of H{sub 2} that can be utilized in fuel cell applications. (author)

  13. Exploration of earth-abundant transition metals (Fe, Co, and Ni) as catalysts in unreactive chemical bond activations.

    Science.gov (United States)

    Su, Bo; Cao, Zhi-Chao; Shi, Zhang-Jie

    2015-03-17

    Activation of inert chemical bonds, such as C-H, C-O, C-C, and so on, is a very important area, to which has been drawn much attention by chemists for a long time and which is viewed as one of the most ideal ways to produce valuable chemicals. Under modern chemical bond activation logic, many conventionally viewed "inert" chemical bonds that were intact under traditional conditions can be reconsidered as novel functionalities, which not only avoids the tedious synthetic procedures for prefunctionalizations and the emission of undesirable wastes but also inspires chemists to create novel synthetic strategies in completely different manners. Although activation of "inert" chemical bonds using stoichiometric amounts of transition metals has been reported in the past, much more attractive and challenging catalytic transformations began to blossom decades ago. Compared with the broad application of late and noble transition metals in this field, the earth-abundant first-row transition-metals, such as Fe, Co, and Ni, have become much more attractive, due to their obvious advantages, including high abundance on earth, low price, low or no toxicity, and unique catalytic characteristics. In this Account, we summarize our recent efforts toward Fe, Co, and Ni catalyzed "inert" chemical bond activation. Our research first unveiled the unique catalytic ability of iron catalysts in C-O bond activation of both carboxylates and benzyl alcohols in the presence of Grignard reagents. The benzylic C-H functionalization was also developed via Fe catalysis with different nucleophiles, including both electron-rich arenes and 1-aryl-vinyl acetates. Cobalt catalysts also showed their uniqueness in both aromatic C-H activation and C-O activation in the presence of Grignard reagents. We reported the first cobalt-catalyzed sp(2) C-H activation/arylation and alkylation of benzo[h]quinoline and phenylpyridine, in which a new catalytic pathway via an oxidative addition process was demonstrated

  14. Excellently reactive Ni/Fe bimetallic catalyst supported by biochar for the remediation of decabromodiphenyl contaminated soil: Reactivity, mechanism, pathways and reducing secondary risks.

    Science.gov (United States)

    Wu, Juan; Yi, YunQiang; Li, YuQing; Fang, Zhanqiang; Tsang, Eric Pokeung

    2016-12-15

    Ni/Fe bimetallic nanoparticles were synthesized using biochar as a support (BC@Ni/Fe) and their effectiveness in removing BDE209 from soil was investigated. BET, SEM, TEM, XPS and FTIR were used to characterize the catalyst, and the efficiencies of biochar, Ni/Fe nanoparticles and BC@Ni/Fe for removing BDE209 from soil were compared. The results showed that Ni/Fe bimetallic nanoparticles highly dispersed in the biochar, reducing its agglomeration. Thus, the reaction activity of BC@Ni/Fe was increased. The removal efficiency of BDE209 by BC@Ni/Fe was 30.2% and 69% higher than that by neat Ni/Fe and biochar, respectively. Meanwhile, an enhanced degradation efficiency of PBDEs in soil was realized by monitoring the formation of Br(-) ions with time in the system. In addition, the degradation products identified by GC-MS showed that the reductive degradation of BDE209 proceeded through stepwise or multistage debromination, for which the degradation pathways and removal mechanisms were speculated. Furthermore, BC@Ni/Fe reduced the bioavailability of metals in soil and adsorbed the degradation products of BDE209, representing an improvement over neat Ni/Fe nanoparticles for the remediation of PBDEs-contaminated soil. Copyright © 2016 Elsevier B.V. All rights reserved.

  15. A Theoretical Investigation on CO Oxidation by Single-Atom Catalysts M1/γ-Al2O3(M=Pd, Fe, Co, and Ni).

    Science.gov (United States)

    Yang, Tao; Fukuda, Ryoichi; Hosokawa, Saburo; Tanaka, Tsunehiro; Sakaki, Shigeyoshi; Ehara, Masahiro

    2017-04-07

    Single-atom catalysts have attracted much interest recently because of their excellent stability, high catalytic activity, and remarkable atom efficiency. Inspired by the recent experimental discovery of a highly efficient single-atom catalyst Pd 1 /γ-Al 2 O 3 , we conducted a comprehensive DFT study on geometries, stabilities and CO oxidation catalytic activities of M 1 /γ-Al 2 O 3 (M=Pd, Fe, Co, and Ni) by using slab-model. One of the most important results here is that Ni 1 /Al 2 O 3 catalyst exhibits higher activity in CO oxidation than Pd 1 /Al 2 O 3 . The CO oxidation occurs through the Mars van Krevelen mechanism, the rate-determining step of which is the generation of CO 2 from CO through abstraction of surface oxygen. The projected density of states (PDOS) of 2 p orbitals of the surface O, the structure of CO-adsorbed surface, charge polarization of CO and charge transfer from CO to surface are important factors for these catalysts. Although the binding energies of Fe and Co with Al 2 O 3 are very large, those of Pd and Ni are small, indicating that the neighboring O atom is not strongly bound to Pd and Ni, which leads to an enhancement of the reactivity of the O atom toward CO. The metal oxidation state is suggested to be one of the crucial factors for the observed catalytic activity.

  16. Influence of Ce-precursor and fuel on structure and catalytic activity of combustion synthesized Ni/CeO{sub 2} catalysts for biogas oxidative steam reforming

    Energy Technology Data Exchange (ETDEWEB)

    Vita, Antonio, E-mail: antonio.vita@itae.cnr.it; Italiano, Cristina; Fabiano, Concetto; Laganà, Massimo; Pino, Lidia

    2015-08-01

    A series of nanosized Ni/CeO{sub 2} catalysts were prepared by Solution Combustion Synthesis (SCS) varying the fuel (oxalyldihydrazide, urea, carbohydrazide and glycerol), the cerium precursor (cerium nitrate and cerium ammonium nitrate) and the nickel loading (ranging between 3.1 and 15.6 wt%). The obtained powders were characterized by X-ray Diffraction (XRD), N{sub 2}-physisorption, CO-chemisorption, Temperature Programmed Reduction (H{sub 2}-TPR) and Scanning Electron Microscopy (SEM). The catalytic activity towards the Oxy Steam Reforming (OSR) of biogas was assessed. The selected operating variables have a strong influence on the nature of combustion and, in turn, on the morphological and structural properties of the synthesized catalysts. Particularly, the use of urea allows to improve nickel dispersion, surface area, particle size and reducibility of the catalysts, affecting positively the biogas OSR performances. - Highlights: • Synthesis of Ni/CeO{sub 2} nanopowders by quick and easy solution combustion synthesis. • The fuel and precursor drive the structural and morphological properties of the catalysts. • The use of urea as fuel allows to improve nickel dispersion, surface area and particle size. • Ni/CeO{sub 2} (7.8 wt% of Ni loading) powders synthesized by urea route exhibits high performances for the biogas OSR process.

  17. Ni/SiO2 Catalyst Prepared with Nickel Nitrate Precursor for Combination of CO2 Reforming and Partial Oxidation of Methane: Characterization and Deactivation Mechanism Investigation

    Directory of Open Access Journals (Sweden)

    Sufang He

    2015-01-01

    Full Text Available The performance of Ni/SiO2 catalyst in the process of combination of CO2 reforming and partial oxidation of methane to produce syngas was studied. The Ni/SiO2 catalysts were prepared by using incipient wetness impregnation method with nickel nitrate as a precursor and characterized by FT-IR, TG-DTA, UV-Raman, XRD, TEM, and H2-TPR. The metal nickel particles with the average size of 37.5 nm were highly dispersed over the catalyst, while the interaction between nickel particles and SiO2 support is relatively weak. The weak NiO-SiO2 interaction disappeared after repeating oxidation-reduction-oxidation in the fluidized bed reactor at 700°C, which resulted in the sintering of metal nickel particles. As a result, a rapid deactivation of the Ni/SiO2 catalysts was observed in 2.5 h reaction on stream.

  18. High Active Zn/Mg-Modified Ni–P/Al2O3 Catalysts Derived from ZnMgNiAl Layered Double Hydroxides for Hydrodesulfurization of Dibenzothiophene

    Directory of Open Access Journals (Sweden)

    Feng Li

    2017-07-01

    Full Text Available A series of ZnMgNiAl layered double hydroxides (LDHs containing 20 wt.% Ni and different Zn/Mg molar ratios were prepared by a coprecipitation method, and then were introduced with H2PO4− via a microwave-hydrothermal method. With the resulting mixtures as the precursors, Zn/Mg-modified ZnMgNi–P/Al2O3 catalysts were prepared. The Zn/Mg molar ratio affected the formation of Ni2P and Ni12P5 in nickel phosphides. The ZnMgNi–P/Al2O3 catalyst with a Zn/Mg molar ratio of 3:1 exhibits the best dibenzothiophene hydrodesulfurization (HDS activity. Compared with the Ni–P/Al2O3 catalyst prepared from the impregnation method, the ZnMgNi–P/Al2O3 catalyst shows a higher HDS activity (81.6% vs. 54.3% and promotes the direct desulfurization of dibenzothiophene.

  19. Hydroconversion of methyl laurate on bifunctional Ni{sub 2}P/AlMCM-41 catalyst prepared via in situ phosphorization using triphenylphosphine

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, Sha; Zhang, Zhena [Tianjin Key Laboratory of Applied Catalysis Science and Technology, Department of Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China); Zhu, Kongying, E-mail: ausky@tju.edu.cn [Analysis and Measurement Center, Tianjin University, Tianjin 300072 (China); Chen, Jixiang, E-mail: jxchen@tju.edu.cn [Tianjin Key Laboratory of Applied Catalysis Science and Technology, Department of Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China)

    2017-05-15

    Highlights: • Bifunctional Ni{sub 2}P/AlMCM-41 was prepared by in situ phosphorization at 300 °C. • There were similar Ni{sub 2}P particle sizes in Ni{sub 2}P/AlMCM-41 with different Si/Al ratios. • The acid amount of Ni{sub 2}P/AlMCM-41 increased with decreasing the Si/Al ratio. • Ni{sub 2}P/AlMCM-41 with the Si/Al ratio of 5 had the highest activity for isomerization. • Ni{sub 2}P/AlMCM-41 had very low activity for methanation and C−C bond hydrogenolysis. - Abstract: A series of Ni{sub 2}P/AlMCM-41-x bifunctional catalysts with different Si/Al ratios (x) were synthesized by in situ phosphorization of Ni/AlMCM-41-x with triphenylphosphine (nominal Ni/P ratio of 0.75) at 300 °C on a fixed-bed reactor. For comparison, NiP/AlMCM-41-5-TPR was also prepared by the TPR method from the supported nickel phosphate with the Ni/P ratio of 1.0, during which metallic Ni rather than Ni{sub 2}P formed. TEM images show that Ni and Ni{sub 2}P particles uniformly distributed in Ni{sub 2}P/AlMCM-41-x and NiP/AlMCM-41-5-TPR. The Ni{sub 2}P/AlMCM-41-x acidity increased with decreasing the Si/Al ratio. In the hydroconversion of methyl laurate, the conversions were close to 100% on all catalysts at 360 °C, 3.0 MPa, methyl laurate WHSV of 2 h{sup −1} and H{sub 2}/methyl laurate ratio of 25. As to Ni{sub 2}P/AlMCM-41-x, with decreasing the Si/Al ratio, the total selectivity to C11 and C12 hydrocarbons decreased, while the total selectivity to isoundecane and isododecane (S{sub i-C11+i-C12}) firstly increased and then decreased. Ni{sub 2}P/AlMCM-41-5 gave the largest S{sub i-C11+i-C12} of 43.2%. While NiP/AlMCM-41-5-TPR gave higher S{sub i-C11+i-C12} than Ni{sub 2}P/AlMCM-41-5, it was more active for the undesired C−C bond cleavage and methanation. We propose that the in-situ phosphorization adopted here is a promising approach to preparing Ni{sub 2}P-based bifunctional catalysts.

  20. A-site-deficiency facilitated in situ growth of bimetallic Ni-Fe nano-alloys: a novel coking-tolerant fuel cell anode catalyst.

    Science.gov (United States)

    Sun, Yi-Fei; Li, Jian-Hui; Cui, Lin; Hua, Bin; Cui, Shao-Hua; Li, Jian; Luo, Jing-Li

    2015-07-07

    To date, most investigations of Ni-Fe bimetallic catalysts for solid oxide fuel cells (SOFCs) have focused on materials with micro-scale particle sizes, which severely restrict their catalytic activity. In this study, we fabricated a Ni- and/or Fe-doped A-site-deficient LaSrCrO3 perovskite (A-LSC) bimetallic anode material on which the in situ exsolution of uniformly dispersed nano Ni, Fe and Ni-Fe alloy with an average particle size of 25 to 30 nm was facilitated by the introduction of A-site deficiency under a reducing atmosphere. The dopants were shown to significantly enhance the electrical conductivity of the material by many orders of magnitude. Further characterization of the bimetallic material showed that the addition of Fe changed the reduction behavior and increased the amount of oxygen vacancies in the material. Fuel cell performance tests demonstrated that the prepared bimetallic anode catalyst with a highly catalytically active nano Ni-Fe alloy promoted the electrochemical performance in 5000 ppm H2S-syngas and improved the carbon deposition resistance compared to a monometallic anode catalyst.

  1. Dry Reforming of Methane on a Highly-Active Ni-CeO2 Catalyst: Effects of Metal-Support Interactions on C-H Bond Breaking.

    Science.gov (United States)

    Liu, Zongyuan; Grinter, David C; Lustemberg, Pablo G; Nguyen-Phan, Thuy-Duong; Zhou, Yinghui; Luo, Si; Waluyo, Iradwikanari; Crumlin, Ethan J; Stacchiola, Dario J; Zhou, Jing; Carrasco, Javier; Busnengo, H Fabio; Ganduglia-Pirovano, M Verónica; Senanayake, Sanjaya D; Rodriguez, José A

    2016-06-20

    Ni-CeO2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO2 at temperatures as low as 300 K, generating CHx and COx species on the surface of the catalyst. Strong metal-support interactions activate Ni for the dissociation of methane. The results of density-functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) to only 0.15 eV on Ni/CeO2-x (111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CHx or C species are detected in the C 1s XPS region. The reforming of methane proceeds in a clean and efficient way. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  2. Synthesis of renewable diesel through hydrodeoxygenation reaction from nyamplung oil (Calophyllum Inophyllum oil) using NiMo/Z and NiMo/C catalysts with rapid heating and cooling method

    Science.gov (United States)

    Susanto, B. H.; Prakasa, M. B.; Shahab, M. H.

    2016-11-01

    The synthesis of metal nanocrystal was conducted by modification preparation from simple heating method which heating and cooling process run rapidly. The result of NiMo/Z 575 °C characterizations are 33.73 m2/gram surface area and 31.80 nm crystal size. By used NiMo/C 700 °C catalyst for 30 minutes which had surface area of 263.21 m2/gram, had 31.77 nm crystal size, and good morphology, obtained catalyst with high activity, selectivity, and stability. After catalyst activated, synthesis of renewable diesel performed in hydrogenation reactor at 375 °C, 12 bar, and 800 rpm. The result of conversion was 81.99%, yield was 68.08%, and selectivity was 84.54%.

  3. 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)

  4. Hierarchical hybrid of Ni{sub 3}N/N-doped reduced graphene oxide nanocomposite as a noble metal free catalyst for oxygen reduction reaction

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, Qi; Li, Yingjun; Li, Yetong [College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021 (China); Huang, Keke [State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012 (China); Wang, Qin, E-mail: qinwang@imu.edu.cn [College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021 (China); Inner Mongolia Key Lab. of Nanoscience and Nanotechnology, Inner Mongolia University, Hohhot 010021 (China); Zhang, Jun, E-mail: cejzhang@imu.edu.cn [College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021 (China); Inner Mongolia Key Lab. of Nanoscience and Nanotechnology, Inner Mongolia University, Hohhot 010021 (China)

    2017-04-01

    Highlights: • Hybrid of Ni{sub 3}N/N-RGO catalysts are synthesized by using a two-step method. • The catalysts manifest superior catalytic activity towards the ORR. • High activities are attributed to enhanced electron density and synergistic effects. - Abstract: Novel nickel nitride (Ni{sub 3}N) nanoparticles supported on nitrogen-doped reduced graphene oxide nanosheets (N-RGOs) are synthesized via a facile strategy including hydrothermal and subsequent calcination methods, in which the reduced graphene oxide nanosheets (RGOs) are simultaneously doped with nitrogen species. By varying the content of the RGOs, a series of Ni{sub 3}N/N-RGO nanocomposites are obtained. The Ni{sub 3}N/N-RGO-30% hybrid nanocomposite exhibits superior catalytic activity towards oxygen reduction reaction (ORR) under alkaline condition (0.1 M KOH). Furthermore, this hybrid catalyst also demonstrates high tolerance to methanol poisoning. The RGO containing rich N confers the nanocomposite with large specific surface area and high electronic conduction ability, which can enhance the catalytic efficiency of Ni{sub 3}N nanoparticles. The enhanced catalytic activity can be attributed to the synergistic effect between Ni{sub 3}N and nitrogen doped reduced graphene oxide. In addition, the sufficient contact between Ni{sub 3}N nanoparticles and the N-RGO nanosheets simultaneously promotes good nanoparticle dispersion and provides a consecutive activity sites to accelerate electron transport continuously, which further enhance the ORR performance. The Ni{sub 3}N/N-RGO may be further an ideal candidate as efficient and inexpensive noble metal-free ORR electrocatalyst in fuel cells.

  5. 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

    , compared to commercial Pt/C (0.22 A mgPt−1). Single-cell performance and electrochemical impedance spectroscopy (EIS) were also tested. The PtNi@Pt catalysts showed enhanced current density of 3.1 A cm−2 at 0.6 V in O2 flow while the commercial Pt/C had the value of 2.5 A cm−2. After 30,000 cycles......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...

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

    Science.gov (United States)

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

    2017-09-01

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

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

    Science.gov (United States)

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

    2014-11-01

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

  8. The role of nano-Ni catalyst in MgH2 obtained by reactive mechanical milling method for solid hydrogen storage application

    Science.gov (United States)

    Jalil, Zulkarnain; Rahwanto, Adi; Handoko, Erfan; Mustanir

    2017-03-01

    Magnesium (Mg) is regarded as one of the candidate material for absorbing hydrogen, because theoretically, has the ability to absorb hydrogen in the large quantities (7.6 wt%). However, Mg has shortage, namely its kinetic reaction is very slow, it takes time to absorb hydrogen at least 60 minutes with very high operating temperatures (300-400°C). The aim of this study is to improve the hydrogen desorption temperature of Mg-based hydrogen storage material. In this work, we used nano-nickel (Ni) as catalyst in MgH2 and obtained by reactive mechanical milling method. The duration of milling was done in 2 hours (soft milling) with the 2 mol% Ni catalyst and milled under hydrogen atmosphere (10 bar). As the results, small amount of 2 mol% Ni in nanometer scale acts as a suitable catalyst for improvement the kinetics of MgH2 which could absorp 5.5 wt% of hydrogen within 10 minutes at 300°C. It is obvious that small amount has much better as catalyst in nanoparticle size and at the same time allowed to reduce the milling process in short time.

  9. Development of Cu and Ni catalysts supported on ZrO{sub 2} for the generation of H{sub 2} by means of the reaction of reformed methanol in atmosphere oxidizer; Desarrollo de catalizadores de Cu y Ni soportados en ZrO{sub 2} para la generacion de H{sub 2} mediante la reaccion de reformado de metanol en atmosfera oxidante

    Energy Technology Data Exchange (ETDEWEB)

    Lopez C, P.

    2012-07-01

    ZrO{sub 2} was prepared by the sol-gel method and calcined at 450 C. The prepared zirconia was impregnated with an aqueous solution of Cu(CH{sub 3}CO{sub 2}){sub 2}{center_dot}H{sub 2}O or NiNO{sub 3}{center_dot}6H{sub 2}O at an appropriate concentration to yield 3 wt % of copper or nickel, respectively, in the mono metallic catalysts. Three bimetallic samples were prepared at 80% Cu and 20% Ni respectively to obtain 3 wt % of total metallic phase. Surface area of the Cu-Ni base catalysts supported on ZrO{sub 2} oxide showed differences as a function of the metal addition. Between them, the Cu/ZrO{sub 2} catalyst had the lowest surface area than other catalysts. X-ray diffraction patterns of the bimetallic catalysts did not show diffraction peaks of the Cu, Ni or bimetallic Cu-Ni alloys. In addition, TPR profiles of the bimetallic catalysts had the lowest reduction temperature compared with the mono metallic samples. The reactivity of the catalysts in the range of 250-350 C showed that the samples prepared by successive impregnation had the highest catalytic activity than the other catalysts studied. Also the selectivity for H{sub 2} production was higher for these catalysts. This finding was associated to the presence of the bimetallic Cu-Ni nanoparticles, as was evidenced by Tem-EDX analysis. (Author)

  10. Influence of Solvent on Liquid Phase Hydrodeoxygenation of Furfural-Acetone Condensation Adduct using Ni/Al2O3-ZrO2 Catalysts

    Science.gov (United States)

    Ulfa, S. M.; Mahfud, A.; Nabilah, S.; Rahman, M. F.

    2017-02-01

    Influence of water and acidic protic solvent on hydrodeoxygenation (HDO) of the furfural-acetone adduct (FAA) over Ni/Al2O3-ZrO2 (NiAZ) catalysts were investigated. The HDO of FAA was carried out in a batch reactor at 150°C for 8 hours. The NiAZ catalysts were home-made catalysts which were prepared by wet impregnation method with 10 and 20% nickel loading. The HDO reaction of FAA using 10NiAZ in water at 150°C gave alkane and oxygenated hydrocarbons at 31.41% with selectivity over tridecane (C13) in 6.67%. On the other hand, a reaction using acetic acid:water (1:19 v/v) in similar reaction condition gave only oxygenated compounds and hydrocracking product (C8-C10). The formation of tridecane (C13) was proposed by hydrogenation of C=O and C=C followed by decarboxylation without hydrocracking process. The presence of water facilitated decarboxylation mechanism by stabilized dehydrogenated derivatives of FAA.

  11. Effects of preparation method on the performance of Ni/Al(2)O(3) catalysts for hydrogen production by bio-oil steam reforming.

    Science.gov (United States)

    Li, Xinbao; Wang, Shurong; Cai, Qinjie; Zhu, Lingjun; Yin, Qianqian; Luo, Zhongyang

    2012-09-01

    Steam reforming of bio-oil derived from the fast pyrolysis of biomass is an economic and renewable process for hydrogen production. The main objective of the present work has been to investigate the effects of the preparation method of Ni/Al(2)O(3) catalysts on their performance in hydrogen production by bio-oil steam reforming. The Ni/Al(2)O(3) catalysts were prepared by impregnation, co-precipitation, and sol-gel methods. XRD, XPS, H(2)-TPR, SEM, TEM, TG, and N(2) physisorption measurements were performed to characterize the texture and structure of the catalysts obtained after calcination and after their subsequent use. Ethanol and bio-oil model compound were selected for steam reforming to evaluate the catalyst performance. The catalyst prepared by the co-precipitation method was found to display better performance than the other two. Under the optimized reaction conditions, an ethanol conversion of 99% and a H(2) yield of 88% were obtained.

  12. Hydrogen Production by Ethanol Steam Reforming (ESR over CeO2 Supported Transition Metal (Fe, Co, Ni, Cu Catalysts: Insight into the Structure-Activity Relationship

    Directory of Open Access Journals (Sweden)

    Michalis Konsolakis

    2016-03-01

    Full Text Available The aim of the present work was to investigate steam reforming of ethanol with regard to H2 production over transition metal catalysts supported on CeO2. Various parameters concerning the effect of temperature (400–800 °C, steam-to-carbon (S/C feed ratio (0.5, 1.5, 3, 6, metal entity (Fe, Co, Ni, Cu and metal loading (15–30 wt.% on the catalytic performance, were thoroughly studied. The optimal performance was obtained for the 20 wt.% Co/CeO2 catalyst, achieving a H2 yield of up to 66% at 400 °C. In addition, the Co/CeO2 catalyst demonstrated excellent stability performance in the whole examined temperature range of 400–800 °C. In contrast, a notable stability degradation, especially at low temperatures, was observed for Ni-, Cu-, and Fe-based catalysts, ascribed mainly to carbon deposition. An extensive characterization study, involving N2 adsorption-desorption (BET, X-ray diffraction (XRD, Scanning Electron Microscopy (SEM/EDS, X-ray Photoelectron Spectroscopy (XPS, and Temperature Programmed Reduction (H2-TPR was undertaken to gain insight into the structure-activity correlation. The excellent reforming performance of Co/CeO2 catalysts could be attributed to their intrinsic reactivity towards ethanol reforming in combination to their high surface oxygen concentration, which hinders the deposition of carbonaceous species.

  13. Metals contamination of aluminosilicate cracking catalysts by Ni- and VO-tetraphenylporphin

    Energy Technology Data Exchange (ETDEWEB)

    Roth, S.A.; Iton, L.E.; Fleisch, T.H.; Meyers, B.L.; Marshall, C.L.; Delgass, W.N.

    1987-11-01

    The interaction of nickel and vanadyl tetraphenylporphin with amorphous silica-alumina, Y zeolite, and a cracking catalyst containing 15% Y zeolite has been studied with a variety of techniques. For the porphins on the silica-alumina and the cracking catalyst, electronic photoacoustic absorption spectrometry, electron paramagnetic resonance on V, X-ray photoelectron spectroscopy, and plasma desorption mass spectrometry confirm interaction of molecularly dispersed porphin molecules with the support but show no demetallation at temperatures below 120/sup 0/C. Since the large porphin molecules cannot fit into the intracrystalline pore structure of the zeolite, the effective loading of those samples was several monolayers. Spectroscopic measurements showed, and scanning electron microscopy confirmed that the porphins form crystallites in this case. Blockage of a substantial portion of the external surface of the zeolite particles was indicated, however, by a large reduction in the measured intracrystalline pore volume after porphin impregnation. Infrared spectroscopy showed that porphin decomposition during calcination in air begins at 200-300/sup 0/C. On the amorphous silica-alumina-containing materials, the decomposition extends over a 150/sup 0/C range during programmed heating. Metal porphins on the zeolite support showed a sharp, apparently catalytic, exotherm and weight loss at a temperature more than 100/sup 0/C higher than that for the onset of loss of molecular structure. These results show that interactions of metal porphins with cracking catalysts and their individual components are a strong function of coverage and that the decomposition of the porphins can be influenced by that interaction. 63 references.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-07-01

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

  15. Synthesis of Highly Branched Polyolefins Using Phenyl Substituted α-Diimine Ni(II Catalysts

    Directory of Open Access Journals (Sweden)

    Fuzhou Wang

    2016-04-01

    Full Text Available A series of α-diimine Ni(II complexes containing bulky phenyl groups, [ArN = C(NaphthC = NAr]NiBr2 (Naphth: 1,8-naphthdiyl, Ar = 2,6-Me2-4-PhC6H2 (C1; Ar = 2,4-Me2-6-PhC6H2 (C2; Ar = 2-Me-4,6-Ph2C6H2 (C3; Ar = 4-Me-2,6-Ph2C6H2 (C4; Ar = 4-Me-2-PhC6H3 (C5; Ar = 2,4,6-Ph3C6H2 (C6, were synthesized and characterized. Upon activation with either diethylaluminum chloride (Et2AlCl or modified methylaluminoxane (MMAO, all Ni(II complexes showed high activities in ethylene polymerization and produced highly branched amorphous polyethylene (up to 145 branches/1000 carbons. Interestingly, the sec-butyl branches were observed in polyethylene depending on polymerization temperature. Polymerization of 1-alkene (1-hexene, 1-octene, 1-decene and 1-hexadecene with C1-MMAO at room temperature resulted in branched polyolefins with narrow Mw/Mn values (ca. 1.2, which suggested a living polymerization. The polymerization results indicated the possibility of precise microstructure control, depending on the polymerization temperature and types of monomers.

  16. Metal (Fe, Co, Ni) supported on different aluminas as Fischer-Tropsch catalyst

    Science.gov (United States)

    Dahlan, Marsih, I. Nyoman; Makertihartha, I. G. B. N.; Praserthdam, Piyasan; Panpranot, Joongjai; Ismunandar

    2015-09-01

    This research aimed to compare the physico-chemical properties of the same metal M (M = iron, cobalt, nickel) supported on aluminas with different morphology and pore size as Fischer-Tropsch catalyst. The aluminas applied as support were alumina synthesized through hydrothermal process, alumina formed by pretreatment of catapal and commercial alumina which named as Ahy, Aca, and Aco respectively. Ahy has uniform morphology of nanotubes while Aca and Aco showed non-uniform morphology of particle lumps. The particle lumps of Aca were larger than those of Aco. Ahy, Aca, and Aco respectively has average pore diameter of 2.75, 2.86 and 2.9 nm. Metals were deposited on the supports by incipient-wetness impregnation method. The catalysts were characterized by XRD, H2-TPR, and H2 chemisorption. Catalyst acitivity test for Fischer-Tropsch reaction was carried out in a micro reactor at 200 °C and 1 atm, and molar ratio of H2/CO = 2:1. The metal oxide particle size increased in the order M/Aco < M/Aca < M/Ahy. The catalysts reducibility also increased according to the order M/Aco < M/Aca < M/Ahy suggesting that the larger metal oxide particles are more reducible. The number of active site was not proportional to the reducibility because during the reduction, larger metal oxide particles were converted into larger metal particles. On the other hand, the number of active sites was inversely proportional to the particle sizes. The number of active site increased in the order M/Ahy < M/Aco < M/Aca. The catalytic activity also increased in the following order M/Ahy < M/Aco < M/Aca. The activity per active site increased according to the order M/Aca < M/Aco < M/Ahy meaning that for M/Ahy, a little increase in active site will lead to a significance increase in catalytic activity. It showed that Ahy has potential for the better support.

  17. Metal (Fe, Co, Ni) supported on different aluminas as Fischer-Tropsch catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Dahlan [Chemistry Education Study Program, Universitas Halu Oleo, Jl. HEA Mokodompit, Kendari 93232 (Indonesia); Marsih, I. Nyoman, E-mail: nyoman@chem.itb.ac.id; Ismunandar [Inorganic and Physical Chemistry Division, Departement of Chemistry, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung 40132 (Indonesia); Makertihartha, I. G. B. N. [Department of Chemical Engineering, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung 40132 (Indonesia); Praserthdam, Piyasan; Panpranot, Joongjai [Center of Excellence on Catalysis and Catalytic Reaction Engineering, Department of Chemical Engineering, Chulalongkorn University, 254 Phayathai Road, Bangkok 10330 (Thailand)

    2015-09-30

    This research aimed to compare the physico-chemical properties of the same metal M (M = iron, cobalt, nickel) supported on aluminas with different morphology and pore size as Fischer-Tropsch catalyst. The aluminas applied as support were alumina synthesized through hydrothermal process, alumina formed by pretreatment of catapal and commercial alumina which named as Ahy, Aca, and Aco respectively. Ahy has uniform morphology of nanotubes while Aca and Aco showed non-uniform morphology of particle lumps. The particle lumps of Aca were larger than those of Aco. Ahy, Aca, and Aco respectively has average pore diameter of 2.75, 2.86 and 2.9 nm. Metals were deposited on the supports by incipient-wetness impregnation method. The catalysts were characterized by XRD, H{sub 2}-TPR, and H{sub 2} chemisorption. Catalyst acitivity test for Fischer-Tropsch reaction was carried out in a micro reactor at 200 °C and 1 atm, and molar ratio of H{sub 2}/CO = 2:1. The metal oxide particle size increased in the order M/Aco < M/Aca < M/Ahy. The catalysts reducibility also increased according to the order M/Aco < M/Aca < M/Ahy suggesting that the larger metal oxide particles are more reducible. The number of active site was not proportional to the reducibility because during the reduction, larger metal oxide particles were converted into larger metal particles. On the other hand, the number of active sites was inversely proportional to the particle sizes. The number of active site increased in the order M/Ahy < M/Aco < M/Aca. The catalytic activity also increased in the following order M/Ahy < M/Aco < M/Aca. The activity per active site increased according to the order M/Aca < M/Aco < M/Ahy meaning that for M/Ahy, a little increase in active site will lead to a significance increase in catalytic activity. It showed that Ahy has potential for the better support.

  18. Radiation-induced synthesis of nanoscale Co- and Ni-based electro-catalysts on carbon for the oxygen reduction reaction.

    Science.gov (United States)

    Soroka, Inna L; Tarakina, Nadezda V; Hermansson, Anton; Bigum, Lukas; Widerberg, Rickard; Andersson, Mikael S; Mathieu, Roland; Paulraj, Alagar R; Kiros, Yohannes

    2017-08-01

    A facile synthesis of 3d-metal based electro-catalysts directly incorporated into a carbon support was carried out by γ-radiation. Transition metals of period 4, i.e. Ni and Co, were precipitated and reduced from their respective salt solutions. The obtained materials were characterized by XRD, SEM, SQUID and the BET methods. Thereafter, the electrodes for fuel cells were fabricated out of synthesized material and their electrochemical performance for the oxygen reduction reaction in 6 M KOH was measured. Although the concentrations of Co and Ni in the electrode material were low (3.4% Co and 0.4% Ni) after reduction by irradiation, both the Ni and Co-based gas diffusion electrodes showed high catalytic activity for oxygen reduction both at room temperature and at 60 °C.

  19. Influences of doping Cr/Fe/Ta on the performance of Ni/CeO{sub 2} catalyst under microwave irradiation in dry reforming of CH{sub 4}

    Energy Technology Data Exchange (ETDEWEB)

    Odedairo, Taiwo [School of Chemical Engineering, The University of Queensland, St Lucia, Brisbane (Australia); Ma, Jun [School of Engineering, University of South Australia, Mawson Lakes, SA (Australia); Chen, Jiuling, E-mail: cjlchen@yahoo.com [School of Chemical Engineering, The University of Queensland, St Lucia, Brisbane (Australia); Wang, Shaobin [Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, WA 6845 (Australia); Zhu, Zhonghua, E-mail: z.zhu@uq.edu.au [School of Chemical Engineering, The University of Queensland, St Lucia, Brisbane (Australia)

    2016-01-15

    The structure of Ni/CeO{sub 2} catalyst with doping of Cr, Fe and Ta was investigated with XRD, N{sub 2} physisorption, XPS and HRTEM and the catalytic activity of the catalysts under microwave irradiation in dry reforming of methane was tested in a microwave reactor. The results show that the introduction of Cr and Ta to Ni/CeO{sub 2} can enhance the interaction between Ni and the support/promoter and inhibit the enlargement of NiO particles during the synthesis. The CH{sub 4} conversions in dry reforming on the catalysts follow the order: Ni/CeO{sub 2}<2Fe–Ni<2Ta–Ni<2Cr–Ni. The superior performance of 2Ta–Ni and 2Cr–Ni may be attributed to the locally-heated Ni particles caused by the strong microwave absorption of the in-situ grown graphene attached on them under microwave irradiation. - Highlights: • The influences of doping Cr, Fe and Ta on Ni/CeO{sub 2} were investigated. • The catalytic performances before and after doping were investigated. • The in-situ grown graphene can promote the conversion of reactants.

  20. CO_2 Methanation Catalysts Prepared from Amorphous Ni-Valve Metal Alloys Containing Platinum Group Elements

    OpenAIRE

    Ken-ichiro, Wakuda; Hiroki, Habazaki; Asahi, Kawashima; Katsuhiko, Asami; Koji, Hashimoto; Institute for Materials Research

    1993-01-01

    The amorphous Ni-valve metal (Ti, Zr, Nb and Ta) alloys containing a few at% of platinum group elements were activated by immersion into hydrofluoric acid and used for hydrogenation of carbon dioxide at 100-300℃. This surface activation led to formation of nanocrystalline surface alloys with high surface area, and to surface enrichment of platinum group elements on the titanium-, niobium- and tantalum-containing alloys, but not on the zirconium-containing alloys. The surface of the latter all...

  1. Synthesis of beaded and entwined carbon nanofibers in Ni:Al alloy catalyst.

    Science.gov (United States)

    Pradhan, Debabrata; Sharon, Maheshwar; Kumar, Mukul; Ando, Yoshinori

    2007-03-01

    This paper reports two new types of carbon nanofibers synthesis by thermal decomposition of n-hexane in presence of Ni-Al alloy in hydrogen atmosphere at 1100 degrees C. One type is "beaded fibers" in which spherical carbon beads (approximately 1 microm) are regularly grown from outer surface of fibers (approximately 0.3 microm). The other new microstructure is "entwined fibers" in which multiple nanofibers of diameter approximately 100 nm grow self-entwined like a braid of hair. Both bead-fiber bonding (in beaded fibers) and fiber-fiber interaction (in entwined fibers) are strong to be detached/unfolded by 30-min ultrasonication.

  2. Kinetics on NiZn Bimetallic Catalysts for Hydrogen Evolution via Selective Dehydrogenation of Methylcyclohexane to Toluene

    KAUST Repository

    Shaikh Ali, Anaam

    2017-01-18

    Liquid organic chemical hydrides are effective hydrogen storage media for easy and safe transport. The chemical couple of methylcyclohexane (MCH) and toluene (TOL) has been considered one of the feasible cycles for a hydrogen carrier, but the selective dehydrogenation of MCH to TOL has been reported using only Pt-based noble metal catalysts. This study reports MCH dehydrogenation to TOL using supported NiZn as a selective, non-noble-metal catalyst. A combined experimental and computational study was conducted to provide insight into the site requirements and reaction mechanism for MCH dehydrogenation to TOL, which were compared with those for cyclohexane (CH) dehydrogenation to benzene (BZ). The kinetic measurements carried out at 300-360°C showed an almost zero order with respect to MCH pressure in the high-pressure region (≥10 kPa) and nearly a positive half order with respective to H pressure (≤40 kPa). These kinetic data for the dehydrogenation reaction paradoxically indicate that hydrogenation of a strongly chemisorbed intermediate originating from TOL is the rate-determining step. Density functional theory (DFT) calculation confirms that the dehydrogenated TOL species at the aliphatic (methyl) position group (CHCH) were strongly adsorbed on the surface, which must be hydrogenated to desorb as TOL. This hydrogen-assisted desorption mechanism explains the essential role of excess H present in the feed in maintaining the activity of the metallic surface for hydrogenation. The rate of the CH to BZ reaction was less sensitive to H pressure than that of MCH to TOL, which can be explained by the absence of a methyl group in the structure, which in turn reduces the binding energy of the adsorbed species. DFT suggests that the improved TOL selectivity by adding Zn to Ni was due to Zn atoms preferentially occupying low-coordination sites on the surface (the corner and edge sites), which are likely the unselective sites responsible for the C-C dissociation of the

  3. Ni-loaded nanocrystalline ceria-zirconia solid solutions prepared via modified Pechini route as stable to coking catalysts of CH4 dry reforming

    Directory of Open Access Journals (Sweden)

    Sadykov Vladislav A.

    2016-01-01

    Full Text Available Mixed nanocrystalline Ce-Zr-O oxides (Ce/Zr = 1 or 7/3 were prepared by modified Pechini route using ethylene glycol solutions of metal salts. Detailed characterization of their real structure and surface properties by X-ray diffraction on synchrotron radiation with the full-profile Rietveld analysis, high resolution electron microscopy with elemental analysis, Raman spectroscopy, UV-Vis and X-ray photoelectron spectroscopy revealed a high homogeneity of cations distribution in nanodomains resulting in stabilization of disordered cubic phase. This provides a high dispersion of NiO loaded on these mixed oxides by wet impregnation, a high reactivity and mobility of oxygen in these catalysts and strong interaction of Ni with support in the reduced state. This helps to achieve a high activity and coking stability of developed catalysts in CH4 dry reforming in feeds with CH4 concentration up to 15% and CH4/CO2 ratio =1.

  4. Yttria-stabilized zirconia (YSZ) supported Ni-Co alloys (precursor of SOFC anodes) as catalysts for the steam reforming of ethanol

    Energy Technology Data Exchange (ETDEWEB)

    Resini, Carlo; Ramis, Gianguido; Busca, Guido [Dipartimento di Ingegneria Chimica e Processo, Universita di Genova, P.le J.F. Kennedy, 1, 16129 Genova and Centro Interuniversitario di Ricerca di Monitoraggio Ambientale (CIMA), via Cadorna, 7, 17100 Savona (Italy); Consorzio INSTM, Via Benedetto Varchi n. 59, 50132 Firenze (Italy); Concepcion Herrera Delgado, Maria; Alemany, Luis J. [Departamento de Ingenieria Quimica, Universidad de Malaga, 29071 Malaga (Spain); Presto, Sabrina; Riani, Paola; Marazza, Rinaldo [Consorzio INSTM, Via Benedetto Varchi n. 59, 50132 Firenze (Italy); Dipartimento di Chimica e Chimica Industriale, Universita di Genova, Via Dodecaneso 31, 16146 Genova (Italy)

    2008-07-15

    Bioethanol is an attractive fuel for direct internal reforming SOFC (DIR-SOFC). The aim of this work is to investigate the activity of Ni-YSZ, used as precursor for the preparation of SOFC anodes and as catalyst of the ethanol steam reforming reaction. The effect of the addition of cobalt is also studied, as the best performance is given by Ni-Co (25:25)/YSZ catalyst. This achieves total conversion of ethanol around 670 K, at which temperature the H{sub 2} yield is 65%. The addition of Co results in the inhibition of the dehydration reaction as well as of methane production. Furthermore, Co also has an effect on the hydrogen yield, by increasing it and thus apparently favouring methane steam reforming. (author)

  5. Hierarchical hybrid of Ni3N/N-doped reduced graphene oxide nanocomposite as a noble metal free catalyst for oxygen reduction reaction

    Science.gov (United States)

    Zhao, Qi; Li, Yingjun; Li, Yetong; Huang, Keke; Wang, Qin; Zhang, Jun

    2017-04-01

    Novel nickel nitride (Ni3N) nanoparticles supported on nitrogen-doped reduced graphene oxide nanosheets (N-RGOs) are synthesized via a facile strategy including hydrothermal and subsequent calcination methods, in which the reduced graphene oxide nanosheets (RGOs) are simultaneously doped with nitrogen species. By varying the content of the RGOs, a series of Ni3N/N-RGO nanocomposites are obtained. The Ni3N/N-RGO-30% hybrid nanocomposite exhibits superior catalytic activity towards oxygen reduction reaction (ORR) under alkaline condition (0.1 M KOH). Furthermore, this hybrid catalyst also demonstrates high tolerance to methanol poisoning. The RGO containing rich N confers the nanocomposite with large specific surface area and high electronic conduction ability, which can enhance the catalytic efficiency of Ni3N nanoparticles. The enhanced catalytic activity can be attributed to the synergistic effect between Ni3N and nitrogen doped reduced graphene oxide. In addition, the sufficient contact between Ni3N nanoparticles and the N-RGO nanosheets simultaneously promotes good nanoparticle dispersion and provides a consecutive activity sites to accelerate electron transport continuously, which further enhance the ORR performance. The Ni3N/N-RGO may be further an ideal candidate as efficient and inexpensive noble metal-free ORR electrocatalyst in fuel cells.

  6. Experimental and theoretical study about sulfur deactivation of Ni/ CeO{sub 2} and Rh/CeO{sub 2} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ocsachoque, Marco A., E-mail: ocmarco@quimica.unlp.edu.ar [Centro de Investigación y Desarrollo en Ciencias Aplicadas “Dr Jorge J. Ronco”, (CONICET, CCT La Plata), Departamento de Química, Facultad de Cs Exactas (UNLP), Calle 48 N° 257, 1900 La Plata (Argentina); Eugenio Russman, Juan I.; Irigoyen, Beatriz [Instituto de Tecnologías del Hidrógeno y Energías Sostenibles (ITHES), Departamento de Ingeniería Química, Facultad de Ingeniería (UBA), Buenos Aires (Argentina); Gazzoli, Delia [Dipartimento di Chimia, Universitá di Roma “La Sapienza”, Roma (Italy); González, María G. [Centro de Investigación y Desarrollo en Ciencias Aplicadas “Dr Jorge J. Ronco”, (CONICET, CCT La Plata), Departamento de Química, Facultad de Cs Exactas (UNLP), Calle 48 N° 257, 1900 La Plata (Argentina)

    2016-04-01

    Sulfur deactivation of Ni/CeO{sub 2} and Rh/CeO{sub 2} catalysts were examined through an experimental and theoretical study. These catalysts were characterized by N{sub 2} adsorption, X-ray diffraction, temperature programmed reaction, thermogravimetric analysis, Uv–visible spectroscopy and Raman spectroscopy, and tested under the methane dry reforming reaction in the presence of H{sub 2}S. On the other hand, different possible interactions of sulfur with Rh, Ni or surface sites of the CeO{sub 2} support were evaluated by performing energy calculations with the density functional theory (DFT). Overall, the results indicate that tolerance to sulfur of Rh/CeO{sub 2} catalyst is higher than that of Ni/CeO{sub 2} one. In this sense, TPR measurements show that reduction of CeO{sub 2} is promoted by the presence of Rh. This effect, probably caused by hydrogen spillover to CeO{sub 2} support during the reduction of RhO{sub x} species, could be linked to a high oxygen donation capacity of Rh/CeO{sub 2} catalysts. Accordingly, the O{sup 2−} species existing on Rh/CeO{sub 2} catalysts, revealed by Raman spectra of these samples, could favor sulfur oxidation and prevent Rh–S interactions. Likewise, the theoretical calculations show that desorption of S–O species from Rh/CeO{sub 2} system is more favorable than that from Ni/CeO{sub 2} one. Therefore, our experimental and theoretical study about sulfur deactivation of Ni and Rh supported on CeO{sub 2} allow us to postulate that Rh can help to desorb SO{sub x} species formed on the support, retarding sulfur poisoning of the Rh/CeO{sub 2} catalysts. - Highlights: • CeO{sub 2} support can act as a sacrifice trap decreasing sulfur poisoning. • Theoretical calculations indicate an important nickel affinity with sulfur. • Rh would favor desorption of S–O species formed on the support. • The O{sup 2−} species present on the Rh–CeO{sub 2} sample favor sulfur removal.

  7. Production of hydrogen with methane decomposition using Ni-Mn/Ce-ZrO{sub 2} catalysts; Produccion de hidrogeno via descomposicion de metano mediante catalizadores de Ni-Mn/Ce-ZrO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Diaz, C.; Hernandez-Pichardo, M.L.; Valenzuela, M. A. [Instituto Politecnico Nacional-ESIQIE, Mexico, D.F. (Mexico)]. E-mail: mhernandezp@ipn.mx; Del Angel, P.; Montoya de la Fuente, J.A. [Instituto Mexicano del Petroleo, Mexico, D.F. (Mexico)

    2009-09-15

    The catalytic decomposition of methane makes it possible to obtain CO and CO{sub 2} free hydrogen, which is a desirable characteristic for fuel cell applications. In addition, this method simultaneously obtains diverse carbon nanostructures with a large variety of applications. This work prepared catalysts with different Ni contents supported by Ce-Zr mixed oxides and doped with manganese to promote activity. The supports were synthesized with surfactant-assisted coprecipitation. The Ni and Mn deposits were performed using conventional impregnation for evaluation in the methane decomposition catalyst at 500 degrees Celsius. It was observed that with the incorporation of 1% of Mn into the Ni0 active phase, the conversion of methane into hydrogen and carbon nanostructures increased. The results of reduction at the programmed temperature indicate that the addition of Mn enables the formation of different NiO{sub x} species, increasing dispersion and the degree of reduction to Ni0. Analyses with electron and transmission microscopy show the formation of distinct species of carbon, including nanotubes, nanofibers and concentric onion-like structures, as well as a significant formation of encapsulated Ni0 particles. [Spanish] La descomposicion catalitica de metano permite la obtencion de hidrogeno libre de CO y CO{sub 2}, lo cual es una caracteristica deseable para su aplicacion en celdas de combustible. Ademas, por esta ruta, simultaneamente se obtienen diversas nanoestructuras de carbono con una gran variedad de aplicaciones. En este trabajo se prepararon catalizadores con diferentes contenidos de Ni soportados en oxidos mixtos Ce-Zr y se doparon con manganeso como promotor de actividad. Los soportes se sintetizaron por coprecipitacion asistida por surfactante y el deposito del Ni y del Mn se efectuo por impregnacion convencional para su evaluacion en la descomposicion catalitica de metano a 500 grados centigrados. Se observo que mediante la incorporacion de 1% de Mn a

  8. Flame synthesis of nanosized Cu-Ce-O, Ni-Ce-O, and Fe-Ce-O catalysts for the water-gas shift (WGS) reaction.

    Science.gov (United States)

    Pati, Ranjan K; Lee, Ivan C; Hou, Sicong; Akhuemonkhan, Osifo; Gaskell, Karen J; Wang, Qi; Frenkel, Anatoly I; Chu, Deryn; Salamanca-Riba, Lourdes G; Ehrman, Sheryl H

    2009-11-01

    A flame synthesis method has been used to prepare nanosized, high-surface-area Cu-Ce-O, Ni-Ce-O, and Fe-Ce-O catalysts from aqueous solutions of metal acetate precursors. The particles were formed by vaporization of the precursors followed by reaction and then gas to particle conversion. The specific surface areas of the synthesized powders ranged from 127 to 163 m(2)/g. High-resolution transmission electron microscope imaging showed that the particle diameters for the ceria materials are in the range of 3-10 nm, and a thin layer of amorphous material was observed on the surface of the particles. The presence and surface enrichment of the transition-metal oxides (CuO, NiO, and Fe(2)O(3)) on the ceria particles were detected using X-ray photoelectron spectroscopy. Electron energy-loss spectroscopic studies suggest the formation of a core-shell structure in the as-prepared particles. Extended X-ray absorption fine structure studies suggest that the dopants in all M-Ce-O systems are almost isostructural with their oxide counterparts, indicating the doping materials form separate oxide phases (CuO, Fe(2)O(3), NiO) within the host matrix (CeO(2)). Etching results confirm that most of the transition-metal oxides are present on the surface of CeO(2), easily dissolved by nitric acid. The performance of the flame-synthesized catalysts was examined toward water-gas shift (WGS) activity for fuel processing applications. The WGS activity of metal ceria catalysts decreases in the order Cu-Ce-O > Ni-Ce-O > Fe-Ce-O > CeO(2) with a feed mixture having a hydrogen to carbon monoxide (H(2)/CO) ratio of 1. There was no methane formation for these catalysts under the tested conditions.

  9. Flame Synthesis of Nanosized Cu-Ce-O, Ni-Ce-O, and Fe-Ce-O Catalysts for the Water-Gas Shift (WGS) Reaction

    Science.gov (United States)

    2009-11-04

    by the flame synthesis method using cerium acetate dissolved in a mixture of acetic acid, 2- butanol , and isooctane (40). In this process, the...gas shift reaction over the Cu-Ce-O, Ni-Ce-O, and Fe-Ce-O catalysts to elu- cidate the catalytic properties of these flame-made ceria- based materials...driven by the system minimizing its surface energy, to form a thermodynamically more stable nanoparticle (42). Therefore, drawing an analogy between

  10. Synthesis and characterization of Ni-CeO{sub 2} catalysts by the hydrothermal method; Sintesis y caracterizacion de catalizadores de Ni-CeO{sub 2} por el metodo hidrotermal

    Energy Technology Data Exchange (ETDEWEB)

    Lazcano O, I.

    2013-07-01

    At the present time the necessity exists to reduce the level of atmospheric pollutants, because these are the main originators of such problems as: the greenhouse effect, acid rain, global heating, among others and that are affecting the human being seriously. In this context, is necessary to look for new solutions that contribute to the improvement of the problems without appealing to limitations in the energy production, because this would imply a non only delay in the economic development, but also in the cultural, technological and of research in our country. An alternative for the energy solution is the use of renewable fuels, because they will decrease the production costs with the time, as well as to diminish the dependence of the fossil fuels, contributing this way to the improvement of the environment quality. The use of the hydrogen as an alternating fuel to the petroleum, is intends as energy solution. The objective of the present work is to develop Ni-CeO{sub 2} catalysts through the hydrothermal method for the hydrogen production starting from the partial oxidation reaction of methanol for the clean fuel generation that does not produce polluting emissions to the environment. As well as, to determine the importance of the metallic load in the catalytic activity for which catalysts to 1 and 2% in weight of Ni were prepared. To achieve these objective different techniques were used to characterize the prepared catalysts, as: Temperature Programmed Reduction to evidence the metal-support interaction, Scanning Electron Microscopy (Sem) to determine the morphology of the catalysts, Surface Area (Bet) with respect to the adsorption-desorption of N{sub 2} and X-Rays Diffraction (XRD) to know the crystalline structure of the catalysts. Also the catalytic properties (activity and selectivity) were studied under the reaction: CH{sub 3}OH + 1/2 O{sub 2} obtaining as products to the CO{sub 2} + 2H{sub 2}, with the help of the multi-tasks equipment Rig-100 that

  11. In Situ Confined Growth Based on a Self-Templating Reduction Strategy of Highly Dispersed Ni Nanoparticles in Hierarchical Yolk-Shell Fe@SiO2 Structures as Efficient Catalysts.

    Science.gov (United States)

    Jiao, Jiao; Wang, Haiyan; Guo, Wanchun; Li, Ruifei; Tian, Kesong; Xu, Zhaopeng; Jia, Yin; Wu, Yuehao; Cao, Ling

    2016-12-19

    Ni-based magnetic catalysts exhibit moderate activity, low cost, and magnetic reusability in hydrogenation reactions. However, Ni nanoparticles anchored on magnetic supports commonly suffer from undesirable agglomeration during catalytic reactions due to the relatively weak affinity of the magnetic support for the Ni nanoparticles. A hierarchical yolk-shell Fe@SiO2 /Ni catalyst, with an inner movable Fe core and an ultrathin SiO2 /Ni shell composed of nanosheets, was synthesized in a self-templating reduction strategy with a hierarchical yolk-shell Fe3 O4 @nickel silicate nanocomposite as the precursor. The spatial confinement of highly dispersed Ni nanoparticles with a mean size of 4 nm within ultrathin SiO2 nanosheets with a thickness of 2.6 nm not only prevented their agglomeration during catalytic transformations but also exposed the abundant active Ni sites to reactants. Moreover, the large inner cavities and interlayer spaces between the assembled ultrathin SiO2 /Ni nanosheets provided suitable mesoporous channels for diffusion of the reactants towards the active sites. As expected, the Fe@SiO2 /Ni catalyst displayed high activity, high stability, and magnetic recoverability for the reduction of nitroaromatic compounds. In particular, the Ni-based catalyst in the conversion of 4-nitroamine maintained a rate of over 98 % and preserved the initial yolk-shell structure without any obvious aggregation of Ni nanoparticles after ten catalytic cycles, which confirmed the high structural stability of the Ni-based catalyst. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Tuning the composition of metastable CoxNiyMg100−xy(OH)(OCH3) nanoplates for optimizing robust methane dry reforming catalyst

    DEFF Research Database (Denmark)

    Fan, Xiaoli; Liu, Zhiting; Zhu, Yi-An

    2015-01-01

    .075Ni7.425Mg92.5O catalyst. The role of Co in the catalyst has been disclosed through kinetic measurements and detailed characterization of the spent catalysts. Co is enriched on the Co–Ni alloy surface under reforming conditions and accelerates the gasification of coke intermediates. Co also enhances...

  13. Nanosized carbon black combined with Ni2O3 as "universal" catalysts for synergistically catalyzing carbonization of polyolefin wastes to synthesize carbon nanotubes and application for supercapacitors.

    Science.gov (United States)

    Wen, Xin; Chen, Xuecheng; Tian, Nana; Gong, Jiang; Liu, Jie; Rümmeli, Mark H; Chu, Paul K; Mijiwska, Ewa; Tang, Tao

    2014-04-01

    The catalytic carbonization of polyolefin materials to synthesize carbon nanotubes (CNTs) is a promising strategy for the processing and recycling of plastic wastes, but this approach is generally limited due to the selectivity of catalysts and the difficulties in separating the polyolefin mixture. In this study, the influence of nanosized carbon black (CB) and Ni2O3 as a novel combined catalyst system on catalyzing carbonization of polypropylene (PP), polyethylene (PE), polystyrene (PS) and their blends was investigated. We showed that this combination was efficient to promote the carbonization of these polymers to produce CNTs with high yields and of good quality. Catalytic pyrolysis and model carbonization experiments indicated that the carbonization mechanism was attributed to the synergistic effect of the combined catalysts rendered by CB and Ni2O3: CB catalyzed the degradation of PP, PE, and PS to selectively produce more aromatic compounds, which were subsequently dehydrogenated and reassembled into CNTs via the catalytic action of CB together with Ni particles. Moreover, the performance of the synthesized CNTs as the electrode of supercapacitor was investigated. The supercapacitor displayed a high specific capacitance as compared to supercapacitors using commercial CNTs and CB. This difference was attributed to the relatively larger specific surface areas of our synthetic CNTs and their more oxygen-containing groups.

  14. Ni-Fe Nitride Nanoplates on Nitrogen-Doped Graphene as a Synergistic Catalyst for Reversible Oxygen Evolution Reaction and Rechargeable Zn-Air Battery.

    Science.gov (United States)

    Fan, Yuchi; Ida, Shintaro; Staykov, Aleksandar; Akbay, Taner; Hagiwara, Hidehisa; Matsuda, Junko; Kaneko, Kenji; Ishihara, Tatsumi

    2017-07-01

    Obtaining bifunctional electrocatalysts with high activity for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is a main hurdle in the application of rechargeable metal-air batteries. Earth-abundant 3d transition metal-based catalysts have been developed for the OER and ORR; however, most of these are based on oxides, whose insulating nature strongly restricts their catalytic performance. This study describes a metallic Ni-Fe nitride/nitrogen-doped graphene hybrid in which 2D Ni-Fe nitride nanoplates are strongly coupled with the graphene support. Electronic structure of the Ni-Fe nitride is changed by hybridizing with the nitrogen-doped graphene. The unique heterostructure of this hybrid catalyst results in very high OER activity with the lowest onset overpotential (150 mV) reported, and good ORR activity comparable to that for commercial Pt/C. The high activity and durability of this bifunctional catalyst are also confirmed in rechargeable zinc-air batteries that are stable for 180 cycles with an overall overpotential of only 0.77 V at 10 mA -2 . © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  15. Catalytic features of Ni/Ba-Ce{sub 0.9}-Y{sub 0.1} catalyst to produce hydrogen for PCFCs by methane reforming

    Energy Technology Data Exchange (ETDEWEB)

    Frontera, P.; Modafferi, V.; Antonucci, P.L. [Dept. of Mechanics and Materials, Mediterranea University, Feo di Vito, 89060 Reggio Calabria (Italy); Frusteri, F.; Bonura, G.; Bottari, M.; Siracusano, S. [CNR-ITAE ' ' Nicola Giordano' ' , via S. Lucia sopra Contesse, 5 - 98126 Messina (Italy)

    2010-10-15

    Methane reforming in steam (SR), auto-thermal (ATR) and partial oxidation (POX) conditions over Ni/Ba-Ce{sub 0.9}-Y{sub 0.1} catalyst was investigated in the temperature range 500-700 C. Catalyst presents a satisfying activity in POX condition only. BCY carrier was not stable in the presence of CO{sub 2} and, irrespective of reaction conditions, it reacts with CO{sub 2} giving rise to the formation of BaCO{sub 3} and CeO{sub 2}. The very low activity observed in SR conditions was due to the negative role exerted by water strongly absorbed on catalyst surface, limiting so the accessibility and reduction state of Ni active sites. In POX condition catalyst is active and satisfying H{sub 2} yield can be reached by operating at T = 700 C. A significant reduction of coke formation was observed by operating in POX at 700 C. On the contrary, in ATR condition at the same reaction temperature huge amount of filamentous coke was observed. (author)

  16. Enhanced photocatalytic efficiency of NiS/TiO{sub 2} composite catalysts using sunset yellow, an azo dye under day light illumination

    Energy Technology Data Exchange (ETDEWEB)

    Rajamanickam, D.; Dhatshanamurthi, P.; Shanthi, M., E-mail: shanthimsm@gmail.com

    2015-01-15

    Highlights: • NiS/TiO{sub 2} was successfully synthesized by sol–gel method. • This new method of preparation gives a homogeneous dispersion of NiS on TiO{sub 2}. • Degradation activity of NiS/TiO{sub 2} is found to be more efficient than other catalysts. • Addition of oxidants enhances the degradation efficiency significantly. • COD measurements reveal the complete mineralization of dye molecules. • The catalyst is found to be reusable. - Abstract: To improve the solar light induced photocatalytic application performances of TiO{sub 2}, in this study, the NiS modified TiO{sub 2} composite photocatalysts with various ratios of NiS to TiO{sub 2} were prepared by sol–gel method. The catalyst was characterized by X-ray diffraction (XRD), high resolution scanning electron microscope (HR-SEM), high resolution transmission electron microscope (HR-TEM), energy dispersive spectra (EDS), diffuse reflectance spectra (DRS), photoluminescence spectra (PL), X-ray photoelectron spectroscopy (XPS), and Brunauer–Emmett–Teller (B–E–T) surface area measurement methods. The photocatalytic activity of NiS/TiO{sub 2} was investigated for the degradation of sunset yellow (SY) in aqueous solution using solar light. The NiS/TiO{sub 2} is found to be more efficient than prepared TiO{sub 2} and TiO{sub 2}–P25 at pH 7 for the mineralization of SY. The effects of operational parameters such as the amount of photocatalyst, dye concentration and initial pH on photo mineralization of SY have been analyzed. The degradation was strongly enhanced in the presence of oxidants such as H{sub 3}K{sub 5}O{sub 18}S{sub 4} (Oxone), KIO{sub 4}, and KBrO{sub 3}. The mineralization of SY has been identified by COD measurements. The catalyst is found to be reusable.

  17. One-Pot Synthesis of Mesoporous Ni-Ti-Al Ternary Oxides: Highly Active and Selective Catalysts for Steam Reforming of Ethanol.

    Science.gov (United States)

    Gonçalves, Alexandre A S; Faustino, Patrícia B; Assaf, José M; Jaroniec, Mietek

    2017-02-22

    One-pot synthesis of nanostructured ternary oxides of Ni, Al, and Ti was designed and performed via evaporation induced self-assembly (EISA). For the purpose of comparison, analogous oxides were also prepared by the impregnation method. The resulting materials were applied in two catalytic reactions: steam reforming of ethanol (SRE) for H2 production (subjected to prior activation with H2) and ethanol dehydration (ED; used without prior activation), to in situ analyze carbon accumulation by ethylene depletion when ethanol interacts with acidic sites present on the support. Modification of Ni-Al mixed oxides with titania was shown to have several benefits. CO2, NH3, and propylamine sorption data indicate a decrease in the strength of acidic and basic sites after addition of titania, which in turn slowed down the carbon accumulation during the ED reaction. These changes in interactions between ethanol and byproducts with the support led to different reaction pathways in SRE, indicating that the catalysts obtained by EISA with titania addition showed higher ethylene selectivity and CO2/CO ratios. The opposite was observed for the impregnated catalysts, which were less coke-stable during ED reactions and showed no ethylene selectivity in SRE. Carbon formed during ED reactions was shown to be thermodynamically less favorable and easier to decompose in the presence of titania. All catalysts studied displayed similar and high selectivities (∼80%) and yields (∼5.3 molH2/molethanol) toward H2, which place them among the most active and selective catalysts for SRE. These results indicate the importance of tailoring the support surface acidity to achieve high reforming performance and higher selectivity toward SRE, one of the key processes to produce cleaner and efficient fuels. For an efficient reforming process, the yield of byproducts is low but still they affect the catalyst stability in the long-run, thus this work may impact future studies toward development of near

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

    Science.gov (United States)

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

    2017-01-01

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

  19. Influence of silica-alumina support ratio on H2production and catalyst carbon deposition from the Ni-catalytic pyrolysis/reforming of waste tyres.

    Science.gov (United States)

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

    2017-10-01

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

  20. Support acidity influence in NiMoS (Nickel and Molybdenum) catalyst for Marlim diesel; Influencia da acidez do suport de catalisadores NiMoS (Niquel e Molibidenio) no hidrotratamento de diesel Marlim

    Energy Technology Data Exchange (ETDEWEB)

    Ferraz, Sheila Guimaraes de Almeida; Zotin, Jose Luiz; Jesus, Anderson Gomes de; Santos, Bruno Martins; Medeiros, Marcus Vinicius Costa [PETROBRAS S.A., Rio de Janeiro, RJ (Brazil). Centro de Pesquisas (CENPES)

    2008-07-01

    The specification of diesel points to the reduction of the sulfur content, of the final boiling point, of the density range and increase of the cetane number. These two last properties are directly related with the ability of the hydrotreating catalytic system in promoting the hydrogenation of aromatic structures and ring opening of the naphthenic compounds, which are both associated to low cetane number. In such way, more acidic catalysts, able to promote the cracking of naphthenic structures, should be evaluated for the diesel HDT. Three bifunctional NiMo catalysts with the same metal content, different acidity and similar active phase dispersion were prepared using alumina, silica-alumina and alumina-Y zeolite as supports. These catalysts were evaluated in a micro-reactor unit for diesel HDT aiming to correlate their activity with the support acidity. The alumina and alumina-zeolite supported catalysts presented better performance than the one supported on silica-alumina. NiMo/alumina-zeolite showed higher cetane and density improvement, associated with a slight decrease in the initial boiling point. (author)

  1. Surface and bulk modifications of 1.5 mole % Sr/La{sub 2}O{sub 3} catalyst with different Co, Ni, and Cu amounts

    Energy Technology Data Exchange (ETDEWEB)

    Gonzalez C, S.L.; Fontal, B.; Moronta, D. [Laboratorio de Cinetica y Catalisis, Departamento de Quimica, Facultad de Ciencias, Universidad de los Andes, Merida 5101A, (Venezuela)

    2001-07-01

    The effects of Co, Ni and Cu oxide content on the surface and bulk of the 1.5 mole % Sr/La{sub 2}O{sub 3} catalysts were studied. Series of M/Sr-La catalysts (MCo, Ni, Cu) were prepared by successive immersion impregnation. The solids were characterized by X-ray diffraction (XRD), infrared spectroscopy (Ftir), temperature-programmed reduction (TPR) electron paramagnetic resonance (EPR) specific surface area measurements (BET) and thermogravimetric analysis (TGA). The Sr/La{sub 2}O{sub 3} modified with different Co, Ni and Cu modified loading shows a strong metal oxide interaction with La{sub 2}O{sub 3}. This probably begins over anionic vacancies or structure defects favoring LaSrMO{sub x} solid solution formation with island-like structures according to a Volmer-Weber growth. It is proposed that the growth mode of La-Co, La-Ni and La-Cu stoichiometric phases occur from solid solutions. The formation of only a La-M single phase, probably non-stoichiometric, increases the material porosity while different phases favor the agglomeration or sintering of the particles. (Author)

  2. In situ grown Ni9S8 nanorod/O-MoS2 nanosheet nanocomposite on carbon cloth as a free binder supercapacitor electrode and hydrogen evolution catalyst

    Science.gov (United States)

    Li, Songzhan; Chen, Tian; Wen, Jian; Gui, Pengbin; Fang, Guojia

    2017-11-01

    Transition metal sulfide nanostructure composites have received significant attention as energy conversion and storage devices. In this work, we report a three-dimension (3D) nanostructure with the Ni9S8 nanorods embedded in oxygen-incorporated MoS2 (O-MoS2) nanosheets for supercapacitors and hydrogen evolution catalysts. The in situ grown Ni9S8/O-MoS2 nanocomposite on carbon cloth can be used as a free binder supercapacitor electrode and hydrogen evolution catalyst. The Ni9S8/O-MoS2 nanocomposite exhibits electrochemical behaviors with a specific capacitance of 907 F g-1 (at 2 A g-1) and good cycle stability after 1200 cycles due to its unique mutual embedding 3D nanostructure. Furthermore, the Ni9S8/O-MoS2 nanocomposite also shows highly electrocatalytic features for hydrogen production with an onset overpotential of ˜150 mV and a low Tafel slope of ˜81 mV dec-1. The oxygen incorporation of MoS2 provides more active sites to participate in the catalytic process for the hydrogen evolution reaction.

  3. 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.

  4. Design of heterogeneous catalysts

    DEFF Research Database (Denmark)

    Frey, Anne Mette

    was inspired by a computational screening, suggesting that alloys such as Ni-Fe, Co-Ni, and Co-Fe should show superior activity to the industrially used nickel catalyst. Especially the Ni-Fe system was considered to be interesting, since such alloy catalysts should be both more active and cheaper than the Ni....... Previously it has been shown that calcination of cobalt catalyst in a NO/He mixture resulted in improved catalytic activity compared to standard air calcined samples, since more homogenous cobalt particles with a narrow particle size distribution were formed. Unfortunately the C5+ selectivity decreased...... well, and the best catalyst prepared had a C5+ yield almost a factor of two higher than a standard air calcined Co catalyst. In the NH3-SCR reaction it is desirable to develop an active and stable catalyst for NOx removal in automotive applications, since the traditionally used vanadium-based catalyst...

  5. Study of CeO₂ Modified AlNi Mixed Pillared Clays Supported Palladium Catalysts for Benzene Adsorption/Desorption-Catalytic Combustion.

    Science.gov (United States)

    Li, Jingrong; Zuo, Shufeng; Yang, Peng; Qi, Chenze

    2017-08-15

    A new functional AlNi-pillared clays (AlNi-PILC) with a large surface area and pore volume was synthesized. The performance of adsorption/desorption-catalytic combustion over CeO 2- modified Pd/AlNi-PILC catalysts was also studied. The results showed that the d 001 -value and specific surface area ( S BET ) of AlNi-PILC reached 2.11 nm and 374.8 m²/g, respectively. The large S BET and the d 001 -value improved the high capacity for benzene adsorption. Also, the strong interaction between PdCe mixed oxides and AlNi-PILC led to the high dispersion of PdO and CeO₂ on the support, which was responsible for the high catalytic performance. Especially, 0.2% Pd/12.5% Ce/AlNi-PILC presented high performance for benzene combustion at 240 °C and high CO₂ selectivity. Also, the combustion temperatures were lower compared to the desorption temperatures, which demonstrated that it could accomplish benzene combustion during the desorption process. Furthermore, its activity did not decrease after continuous reaction for 1000 h in dry air, and it also displayed good resistance to water and the chlorinated compound, making it a promising catalytic material for the elimination of volatile organic compounds.

  6. Parametric study of the decomposition of methane using a NiCu/Al{sub 2}O{sub 3} catalyst in a fluidized bed reactor

    Energy Technology Data Exchange (ETDEWEB)

    Pinilla, J.L.; Suelves, I.; Lazaro, M.J.; Moliner, R. [Instituto de Carboquimica, CSIC, Miguel Luesma Castan 4, 50018 Zaragoza (Spain); Palacios, J.M. [Instituto de Catalisis y Petroleoquimica, CSIC, Campus Universidad Autonoma, Cantoblanco, 28049 Madrid (Spain)

    2010-09-15

    CO{sub 2}-free production of hydrogen via catalytic decomposition of methane (CDM) was studied in a fluidized bed reactor (FBR) using a NiCu/Al{sub 2}O{sub 3} catalyst. A parametric study of the effects of some process variables, including catalyst particle size, reaction temperature, space velocity and the ratio of gas flow velocity to the minimum fluidization velocity (u{sub o}/u{sub mf}), was undertaken. A mean particle size of 150 {mu}m allows optimization of results in terms of hydrogen production without agglomeration problems. The operating conditions strongly affect the catalyst performance: hydrogen production was enhanced by increasing operating temperature and lowering space velocity. However, increases in operating temperature, space velocity and the ratio u{sub o}/u{sub mf} provoked increases in the catalyst deactivation rate. At 700 C, carbon was deposited as carbon nanofibers, while higher temperatures promoted the formation of encapsulating carbon, which led to rapid catalyst deactivation. (author)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1996-10-28

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

  8. Steam reforming of bio-ethanol over Ni on Ce-ZrO2 support: Influence of redox properties on the catalyst reactivity

    Directory of Open Access Journals (Sweden)

    Sumittra Charojrochkul

    2006-11-01

    Full Text Available The steam reforming of ethanol over Ni on Ce-ZrO2 support, (Ni/ Ce-ZrO2 were studied. The catalyst provides significantly higher reforming reactivity and excellent resistance toward carbon deposition compared to Ni/Al2O3 under the same conditions. At the temperature above 800ºC, the main products from the reforming processes over Ni/Ce-ZrO2 were H2, CO, and CO2 with small amount of CH4 depending on the inlet ethanol/steam and oxygen/ethanol ratios, whereas high hydrocarbon compounds i.e., C2H4 and C2H6 were also observed from the reforming of ethanol over Ni/Al2O3 in the range of conditions studied (700- 1000ºC.These excellent ethanol reforming performances of Ni/Ce-ZrO2 in terms of stability, reactivity and product selectivities are due to the high redox property of Ce-ZrO2. During the ethanol reforming process, in addition to the reactions on Ni surface, the gas-solid reactions between the gaseous components presented in the system (C2H5OH, C2H6, C2H4, CH4, CO2, CO, H2O, and H2 and the lattice oxygen (Ox on Ce-ZrO2 surface also take place. Among these redox reactions, the reactions of adsorbed surface hydrocarbons with the lattice oxygen (Ox (CnHm + Ox → nCO + m/2(H2 + Ox-n can eliminate the formation of high hydrocarbons (C2H6 and C2H4, which easily decompose and form carbon species on Ni surface (CnHm→ nC + m/2H2.

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

    Science.gov (United States)

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

    2018-02-01

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

  10. Ni-Co nanoparticles immobilized on a 3D Ni foam template as a highly efficient catalyst for borohydride electrooxidation in alkaline medium

    Science.gov (United States)

    Guo, Meisong; Cheng, Yu; Yu, Yanan; Hu, Jingbo

    2017-09-01

    Proton exchange membrane (PEM) fuel cells have drawn a great deal of attention due to the rapidly growing energy consumption. Recently, Ni- and Co-based materials have been considered as promising electorcatalysts owing to their multi-functionality. In this work, Ni and Co nanoparticles are directly immobilized on a three-dimensional Ni foam substrate (Ni-Co/NF) without any conductive agents or polymer binder by a facile ion implantation method. The structure and morphology of the Ni-Co/NF electrode were characterized by scanning electron microscopy, powder X-ray diffraction, and X-ray photoelectron spectroscopy. The performance of the Ni-Co/NF electrode in the electrochemical oxidation of NaBH4 is investigated by cyclic voltammetry and chronoamperometry. The Ni-Co/NF electrode exhibited excellent electrocatalytic activity and good stability during electrochemical reactions. These properties are attributed to the 3D porous structure of the Ni foam and the synergistic effect of Ni and Co nanoparticles. The enhanced electrocatalytic performance in NaBH4 electrooxidation compared with either Ni or Co nanoparticles alone suggests that the Ni-Co/NF is promising for fuel cell applications.

  11. The synergistic effect of catalysts on hydrogen desorption properties of MgH2–TiO2–NiO nanocomposite

    Directory of Open Access Journals (Sweden)

    Farshad Rajabpour

    2016-10-01

    Full Text Available Abstract The high desorption temperature and slow desorption kinetics of MgH2 makes it less competitive for future mobile applications; using a catalyst accompanied by mechanical milling seems to be a good solution to overcome those problems. Therefore, the addition of TiO2 and NiO to MgH2 accompanied by 15 h of mechanical milling was considered in this study. The phase constituent and hydrogen desorption of the powder mixture were investigated using X-ray diffraction (XRD and a Sievert-type apparatus, respectively. XRD results showed that after milling, no binary or ternary compounds were formed, but hydrogen desorption time decreased and the desorbed hydrogen content increased. It seems that the increase in desorbed hydrogen was related to the simultaneous catalytic effect of TiO2 and NiO as well as mechanical milling. The results showed that the addition of both catalysts can improve the hydrogen desorption behavior of MgH2-based nanocomposite compared to the addition of only one catalyst of the same amount.

  12. Effect of WO{sub x} on Co and Ni/Hydrotalcite catalysts to obtain hydrogen from bioethanol; Efecto del WO{sub x} sobre catalizadores de Co, Ni/hidrotalcita para obtener hidrogeno a partir de bioetanol

    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

    This work studies the effect of tungsten oxides on the synthesis, characterization and reaction of Co catalysts, Ni exchanges in hydrotalcite, to produce H{sub 2} from ethanol. The catalysts were characterized by 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 450 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. Other findings include a pore morphology in the form of parallel plates and a mesoporous distribution (bimodal) with areas of 150-250 m{sup 2}/g. Infrared OH vibrations found, H{sub 2}O, Al-OH, Mg-and CO32-OH, also a low intensity peak related to vibration of type W = O. For Raman found links the W-O-W. UV-vis a band was found in the ultraviolet region, which in the case of the series of cobalt decreases as the content of W. The opposite occurred for the series of Ni. W was observed that promotes the conversion of Co in the range up to 80% while not promoted in the case of Ni. W showed that promotes catalyst stability (after 430 min), Co series showed a conversion of 80% and reached 90% Ni, no catalyst was deactivated before 350 min. [Spanish] En este trabajo se estudia el efecto de los oxidos de tungsteno en la sintesis, caracterizacion y reaccion de catalizadores de Co, Ni intercambiados en hidrotalcita, para la produccion de H{sub 2} a partir de etanol. Los catalizadores se caracterizaron por area BET, difraccion de rayos X, espectroscopias: Raman, Infrarrojo y UV-vis. La evaluacion catalitica se llevo a cabo en un equipo de microrreaccion usando una relacion agua/etanol de 4 a 450 grados centigrados se estudio el efecto del contenido de W desde 0.5 hasta 3%. La difraccion de rayos X para las series de Co y Ni mostro una disminucion continua de la cristalinidad conforme aumento el contenido de W

  13. Cracking vegetable oil from Callophylluminnophyllum L. seeds to bio-gasoline by Ni-Mo/Al2O3 and Ni-Mo/Zeolite as micro-porous catalysts

    Science.gov (United States)

    Savitri, Effendi, R.; Tursiloadi, S.

    2016-02-01

    Natural minerals such as zeolite are local natural resources in the various regions in Indonesia. Studies on the application of natural mineral currently carried out by national research institutions, among others, as a filler, bleaching agent, or dehydration agent. However, not many studies that utilize these natural minerals as green catalysts material which has high performance for biomass conversion processes and ready to be applied directly by the bio-fuel industry. The trend movement of green and sustainable chemistry research that designing environmentally friendly chemical processes from renewable raw materials to produce innovative products derived biomass for bio-fuel. Callophylluminnophyllum L. seeds can be used as raw material for bio-energy because of its high oil content. Fatty acid and triglyceride compounds from this oil can be cracked into bio-gasoline, which does not contain oxygen in the hydrocarbon structure. Bio-gasoline commonly is referred to as drop-in biofuel because it can be directly used as a substitute fuel. This paper focused on the preparation and formulation of the catalyst NiMo/H-Zeolite and Ni-Mo/Al2O3 which were used in hydro-cracking process of oil from Callophylluminnophyllum L. seeds to produce bio-gasoline. The catalysts were analyzed using XRD, BET and IR-adsorbed pyridine method. The results of hydro-cracking products mostly were paraffin (C10-C19) straight chain, with 59.5 % peak area based on GC-MS analysis.

  14. Electronic Structure and Reactivity of TM-Doped La1-xSrxCoO3 (TM=Ni, Fe Heterogeneous Catalysts

    Directory of Open Access Journals (Sweden)

    S. A. Jones

    2001-11-01

    Full Text Available The catalytic properties of LaCoO3 in aqueous oxidation are explored as a function of doping. Both Sr substitution for La and Fe/Ni substitution for Co are studied. The reaction of interest is the aqueous epoxidation of crotyl alcohol with hydrogen peroxide. The reaction products are measured using GC, and the decomposition of hydrogen peroxide is studied using the volume of oxygen evolved during reaction. Strong variations in the activity to epoxide formation are observed, with Fe-doped samples being rather inactive in the reaction. SR VUV photoemission is used to explore the surface reactivity of the ceramic catalysts in aqueous solution, using H2O as a probe molecule. These measurements are complemented by XANES measurements designed to probe the local defect structure and XPS measurements of surface composition. We relate the observed catalytic activity to the defect structure of the doped materials. In Ni-doped materials, oxygen vacancies appear to be the predominant defect, whereas in Fe-doped samples, electron holes are stabilized on Fe, leading to very different catalytic behaviour. Surface studies in combination with AA measurements reveal some dissolution of the catalyst into solution during the reaction. The surface reactivity to water is influenced by the TM d electron count, with water binding more strongly to Fe-doped materials than to those containing Ni. The influence of these factors on the rate of the unwanted hydrogen peroxide decomposition reaction and hence on activity in epoxidation is discussed.

  15. Synthesis and characterization of Fe–Ni/ɣ-Al2O3 egg-shell catalyst for H2 generation by ammonia decomposition

    DEFF Research Database (Denmark)

    Silva, Hugo José Lopes; Nielsen, Morten Godtfred; Fiordaliso, Elisabetta Maria

    2015-01-01

    of the active phase should match with the type of reaction. In this work, a novel synthesis route was developed for the preparation of a Fe–Ni/ɣ-Al2O3 egg-shell catalyst. Egg-shell is a preferred profile considering the highly endothermic nature of ammonia decomposition reaction. The high viscosity of glycerol......-EDX) and optical microscopy. A three-dimensional (3-D) reconstruction of the spherical-shaped ɣ-Al2O3 was achieved using X-ray micro tomography and the Fe–Ni egg-shell spatial distribution was inspected throughout the entire volume of the support body. Transmission electron microscopy (TEM) specimen preparation...... using focused ion bean (FIB) milling allowed to acquire high resolution images of the Ni and Fe nanoparticles on ɣ-Al2O3, which is particularly challenging due to the crystalline nature of this support. Distinct regions of the egg-shell catalyst were analyzed through scanning TEM (STEM) and TEM...

  16. Ni/γ-Al2O3 Catalyst for CO2 Reforming of Benzene as a Model Compound of Biomass Gasification Tar: Promotional Effect of Ultrasonic Treatment on Catalytic Performance

    Science.gov (United States)

    Li, B.; Chen, H. P.; Yang, H. P.; Yang, G. L.; Wang, X. H.; Zhang, S. H.

    This paper aims to understand the promotional effect of ultrasonic treatment on catalytic performance of Ni/γ-Al2O3 catalyst for CO2 reforming of benzene as a model compound of tar derived from biomass gasification, and the catalytic cracking mechanism was also discussed. Firstly, three Ni/γ-Al2O3catalysts were prepared by ultrasonic impregnation as the ultrasonic power variantat0, 120 and 500W, andthephysicochemical property of catalysts were characterized using N2-adsorption, SEM and XRD, etc. Then the catalytic performance of three catalysts for CO2 reforming of benzene wastestedin amicro-reactor.Theoutlet gaswas measured using a Micro-GC. Finally, the coking amount on the catalyst surface was measured by thermogravimetry (TG). The results showed that ultrasonic treatment significanüy modified the pore size distribution of the catalysts especiallyin theporesize range of 10-50nm andalso improved the capability of the coke resistance. It's beneficial to increase the lifetime of the catalyst. Meanwhile, lower ultrasonic power(120W) was more favorableto improve the coke resistance of the catalyst in the power range tested (120 and 500W). The main surface reactions over Ni/γ-Al2O3 catalysts included two steps: Firstly, benzeneadsorbed on the catalyst surface, the metal active sites dehydrogenation took place, and the residual molecule fragments (coke precursor) wouldcondense further which led to coke formation.Then, CO2 reacted with coke precursor and coke for coke elimination. The first step carriedout very quickly, and the second step was the rate-determining step.To reduce the cokedeposition on the catalyst surface, the performance of CO2 adsorption and activation and surface oxygen transmission capacity should be improved further.

  17. Hydrogen-Rich Gas Production by Sorption Enhanced Steam Reforming of Woodgas Containing TAR over a Commercial Ni Catalyst and Calcined Dolomite as CO2 Sorbent

    Directory of Open Access Journals (Sweden)

    Vincenzo Naso

    2013-07-01

    Full Text Available The aim of this work was the evaluation of the catalytic steam reforming of a gaseous fuel obtained by steam biomass gasification to convert topping atmosphere residue (TAR and CH4 and to produce pure H2 by means of a CO2 sorbent. This experimental work deals with the demonstration of the practical feasibility of such concepts, using a real woodgas obtained from fluidized bed steam gasification of hazelnut shells. This study evaluates the use of a commercial Ni catalyst and calcined dolomite (CaO/MgO. The bed material simultaneously acts as reforming catalyst and CO2 sorbent. The experimental investigations have been carried out in a fixed bed micro-reactor rig using a slipstream from the gasifier to evaluate gas cleaning and upgrading options. The reforming/sorption tests were carried out at 650 °C while regeneration of the sorbent was carried out at 850 °C in a nitrogen environment. Both combinations of catalyst and sorbent are very effective in TAR and CH4 removal, with conversions near 100%, while the simultaneous CO2 sorption effectively enhances the water gas shift reaction producing a gas with a hydrogen volume fraction of over 90%. Multicycle tests of reforming/CO2 capture and regeneration were performed to verify the stability of the catalysts and sorbents to remove TAR and capture CO2 during the duty cycle.

  18. Removal of Bismarck Brown G Dye from Simulated Industrial Wastewaters over (Co, Ni3O4/Al2O3 Co- Catalyst

    Directory of Open Access Journals (Sweden)

    Emman J. Mohammad

    2017-02-01

    Full Text Available The spinel co- catalyst (Co, Ni3O4/Al2O3 was prepared using co-precipitation method. The produced material then was calcinated at temperature (600 ᵒC for 4 hours. The resultant catalysts were characterized using powder X-rays diffraction (PXRD, Fourier transform infrared spectroscopy (FTIR. The photocatalytic activity and the adsorption ability of these materials were investigated by following photocatalytic degradation and adsorption of Bismarck braown G dyes (BBG from simulated industrial wastewaters. Different reaction parameters and conditions were undertaken, including studying the effect of pH of the solution, the amount of the used catalyst, and the effect of temperature. In addition to that both of Frundlich and Langmuir adsorption isotherms were studied. From the obtained results in this study, it was found that the best efficiency for BBG removal was around 92.4%. This was achieved at optimal reaction conditions which were PH =3, weight of the catalyst 0.2g and time of reaction was one hour.

  19. 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)

  20. Surface and bulk modifications of 1.5 mole % Sr/La{sub 2}O{sub 3} catalyst with different Co, Ni, and Cu amounts

    Energy Technology Data Exchange (ETDEWEB)

    Gonzalez Cortes, Sergio; Fontal, Bernardo [Universidad de los Andes, Merida (Venezuela); Moronta, Delfin [Universidad Central de Venezuela, Caracas (Venezuela)

    2001-08-01

    The effects of Co, Ni and Cu oxide content on the surface and bulk of the 1.5 mole % Sr/La{sub 2}O{sub 3} catalysts were studied. Series of M/Sr-La catalysts (MCo, Ni, Cu) were prepared by successive immersion impregnation. The solids were characterized by X-ray diffraction (XRD), infrared spectroscopy (FTIR), temperature-programmed reduction (TPR), electron paramagnetic resonance (EPR), specific surface area measurements (BET) and thermogravimetric analysis (TGA). The Sr/La{sub 2}O{sub 3} modified with different Co, Ni, and Cu loading shows a strong metal oxide interaction with La{sub 2}O{sub 3}. This probably begin over anionic vacancies or structure defects favoring LaSrMO{sub x} solid solution formation with island-like structures according to a Volmer-Weber growth. It is proposed that the growth mode of La-Co, La-Ni and La-Cu stoichiometric phases occur from solid solutions. The formation of only a La-M single phase, probably non-stoichiometric, increases the material porosity while different phases favor the agglomeration or sintering of the particles. [Spanish] En este trabajo se estudia el efecto de la cantidad de cobalto, niquel y cobre sobre las estructuras superficial y masica del sistema 1.5% molar Sr/La{sub 2}O{sub 3}. Los catalizadores M/Sr-La (M = Co, Ni, Cu) fueron preparados por el metodo de impregnacion con exceso de solucion. Los solidos se caracterizaron por difraccion de rayos-X, espectroscopia infrarroja con transformada de Fourier, reduccion a temperatura programada, resonancia paramagnetica del electron, medidas del area superficial especifica por el metodo de BET y analisis termogravimetrico. El catalizador Sr/La{sub 2}O{sub 3} modificado con diferentes cantidades de Co, Ni y Cu muestra una interaccion fuerte con el oxido del metal de transicion, probablemente sobre las vacancias anionicas o defectos estructurales que favorecen la formacion de la solucion solida LaSrMox en forma de isla, segun el mecanismo de crecimiento de fase de Volmer

  1. Activation and regeneration of a NiMo/Al[sub 2]O[sub 3] hydrotreatment catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Teixeira da Silva, V.L.S.; Schmal, M. (Univ. Federal, Rio de Janeiro (Brazil)); Frety, R. (CNRS, Villeurbanne (France). Inst. de Reserches sur la Catalyse)

    1994-07-01

    Activation and regeneration procedures applied to a nickel-molybdenum on alumina catalyst, both fresh and spent, were tested by the hydrodesulfurization of thiophene. Characterization techniques used included temperature programmed reduction and oxidation (TPR,TPO), diffuse reflectance spectroscopy (DRS), and X-ray diffraction (XRD). The fresh catalyst was treated by sulfiding, reoxidation, and resulfiding. This sequence was found to be more effective than one sulfiding step, possibly because of the formation of a nickel molybdate phase during reoxidation. The spent catalyst could not be regenerated completely although its original surface properties were attained. The loss of activity of the spent catalysts was alluded by TPO to result from nickel-molybdenum segregation which probably happened because of the excessive heat from burning the coke present on the catalyst.

  2. Ni2+ supported on hydroxyapatite-core@shell γ-Fe2O3 nanoparticles as new and green catalyst for the synthesis of 3,4-dihydropyrimidin-2(1H-ones under solvent-free condition

    Directory of Open Access Journals (Sweden)

    Eshagh Rezaee Nezhad

    2013-10-01

    Full Text Available The aim of this research is to study Ni2+ supported on hydroxyapatite-core-shell magnetic γ-Fe2O3 nanoparticles (γ-Fe2O3@HAp-Ni2+ as a green and recyclable catalyst for the Biginelli reaction under solvent-free conditions. One-pot multi-component condensation of 1,3-dicarbonyl compounds, urea and aldehydes at 80 oC affords the corresponding compounds in high yields and in short reaction times using γ-Fe2O3@HAp-Ni2+. The catalyst can be readily isolated using an external magnet and no obvious loss of activity was observed when the catalyst was reused in seven consecutive runs. The mean size and the surface morphology of the nanoparticles were characterized by transmission electron microscopy, scanning electron microscope, vibrating sample magnetometry, X-ray powder diffraction and Fourier transform infrared techniques.

  3. Produção de hidrogênio a partir da reforma a vapor de etanol utilizando catalisadores Cu/Ni/gama-Al2o3 Hydrogen production by ethanol steam reforming using Cu/Ni/gamma-Al2o3 catalysts

    Directory of Open Access Journals (Sweden)

    Thaísa A. Maia

    2007-04-01

    Full Text Available Cu/Ni/gamma-Al2O3 catalysts were prepared by an impregnation method with 2.5 or 5% wt of copper and 5 or 15% wt of nickel and applied in ethanol steam reforming. The catalysts were characterized by atomic absorption spectrophotometry, X-ray diffraction, temperature programmed reduction with hydrogen and nitrogen adsorption. The samples showed low crystallinity, with the presence of CuO and NiO, both as crystallites and in dispersed phase, as well as of NiO-Al2O3. The catalytic tests carried out at 400 ºC, with a 3:1 water/ethanol molar ratio, indicated the 5Cu/5Ni/Al2O3 catalyst as the most active for hydrogen production, with a hydrogen yield of 77% and ethanol conversion of 98%.

  4. Session 4: Combine reforming of methane over LaCo{sub 1-x}Ni{sub x}O{sub 3} perovskites as catalysts precursors

    Energy Technology Data Exchange (ETDEWEB)

    Goldwasser, M.R.; Lugo, M.L.; Rivas, M.E.; Pietri, E.; Perez-Zurita, M.J.; Cubeiro, M.L. [Centro de Catalisis, Petroleo y Petroquimica, Escuela de Quimica, Fac. Ciencias, UCV, Apartado 47102, Los Chaguaramos, Caracas (Venezuela); Griboval-Constant, A.; Leclercq, G. [Universite des Sciences ET Technologies de Lille, Lab. de Catalyse Heterogene et Homogene, 59 - Villeneuve D' Ascq (France)

    2004-07-01

    The effect of the partial and total substitution of the nickel by cobalt in a LaNiO{sub 3} perovskite as catalyst precursors in the combine reforming of methane with CO{sub 2} and O{sub 2} for the production of syngas was studied. The solids were synthesized by the sol gel method and characterized by IR, BET surface area, XRD, TPR, EDX and in situ XRD under the condition of fresh, reduced and used samples. The results showed that through this synthesis it is possible to obtain highly crystalline, homogeneous and pure solids, with well-defined structures. It was observed that by reduction of the perovskites, the metals (Co, Ni) are in a highly disperse state on a matrix compose of the La{sub 2}O{sub 3}. The stabilization of nickel by the presence of Co was evidenced, decreasing deactivation by avoiding the sintering of metals by coke formation on the surface of the catalysts. (authors)

  5. Total oxidation of benzene over ACo2O4 (A = Cu, Ni and Mn) catalysts: In situ DRIFTS account for understanding the reaction mechanism

    Science.gov (United States)

    Wang, Xiuyun; Zhao, Weitao; Wu, Xiangwei; Zhang, Tianhua; Liu, Yi; Zhang, Kai; Xiao, Yihong; Jiang, Lilong

    2017-12-01

    Mesoporous ACo2O4 (A = Cu, Ni and Mn) catalysts with high surface area were synthesized by a simple co-nanocasting approach using SBA-15 as a hard template. Their catalytic performances for total oxidation of benzene were tested and physicochemical properties were characterized in detail by means of XRD, N2 physisorption, TEM/HR-TEM, XPS, H2-TPR, O2-TPD-MS and in situ DRIFTS. The results demonstrate that benzene conversion in MnCo2O4 is more than 90% at 238 °C, which is higher than that of NiCo2O4 and CuCo2O4. The superior catalytic activity in MnCo2O4 is associated with its highly ordered mesoporous structure, higher surface Mn concentration and more active oxygen species. In situ DRIFTS results indicate that the lattice oxygen species are participated in the generation of carboxylates intermediate species over ACo2O4, while the surface active oxygen species favor the oxidation of carboxylates species to final products. All the results indicate that the oxidation of benzene in ACo2O4 catalysts consist of MvK and L-H mechanisms.

  6. Effect of CO{sub 2}-admixture on the catalytic performance of Ni-Nb-M-O catalysts in oxidative dehydrogenation of ethane to ethylene

    Energy Technology Data Exchange (ETDEWEB)

    Qiao, A.; Kalevaru, V.N.; Martin, A. [Rostock Univ. (Germany). Leibniz-Institut fuer Katalyse e.V.; Hari Kumar, A. Sri; Lingaiah, N.; Prasad, P.S. Sai [Indian Institute of Chemical Technology, Hyderabad (India). Inorganic and Physical Chemistry Div.

    2012-07-01

    In this work, we report the synthesis, characterization and application of Ni-Nb-M-O catalysts with different promoters (M = Cr, Mo, W) for the oxidative dehydrogenation (ODH) of ethane to ethylene. Ni:Nb:M ratio was kept at 1:0.176:0.1 (atomic ratio). The catalysts were calcined at 450 C/5h/air. Catalytic tests were carried out in a fixed bed quartz reactor in the temperature range from 300 to 450 C, with a fixed W/F (1.02 g/cm{sup 3} . s{sup -1}) but with changing mole ratios of C{sub 2}H{sub 6}:O{sub 2}:CO{sub 2}:N{sub 2} (1:0-1.4:1.4-0:2). The product analysis was made off-line using GC equipped with FID. It is evident that the CO{sub 2}-admixture to the reactant feed caused a slight decrease in the conversion of ethane but considerably improved the selectivity of ethylene. Among the three promoters of the same group applied, Cr exhibited superior performance compared to other two. This means increase in d-character of transition metal (i.e. from 3d to 5d) has shown an adverse effect on the conversion of ethane and selectivity of ethylene. (orig.)

  7. Ethanol steam reforming over Ni/M{sub x}O{sub y}-Al{sub 2}O{sub 3} (M=Ce, La, Zr and Mg) catalysts: Influence of support on the hydrogen production

    Energy Technology Data Exchange (ETDEWEB)

    Sanchez-Sanchez, M.C.; Navarro, R.M.; Fierro, J.L.G. [Instituto de Catalisis y Petroleoquimica, CSIC, C/ Marie Curie 2 Cantoblanco 28049 Madrid (Spain)

    2007-07-15

    Hydrogen production from ethanol reforming over alumina-supported nickel catalysts modified with Ce, Mg, Zr and La was studied. Characterization of catalysts by XRD, TPR, XRD and TPD of NH{sub 3} revealed changes in the acidity, nickel dispersion and nickel-support interaction with the type of the modifier added to Al{sub 2}O{sub 3}. The acidity of catalysts containing Mg, Ce, La and Zr additives decreased with respect to that supported on bare Al{sub 2}O{sub 3}. The trend of metal dispersion as derived from XRD and H{sub 2} chemisorption results followed the order: La{sub 2}O{sub 3}-Al{sub 2}O{sub 3}>MgO-Al{sub 2}O{sub 3}>CeO{sub 2}-Al{sub 2}O{sub 3}>Al{sub 2}O{sub 3}>ZrO{sub 2}-Al{sub 2}O{sub 3}. TPR and XPS analyses indicate the development of strong interactions between nickel species and ZrO{sub 2}, La{sub 2}O{sub 3} and CeO{sub 2} oxides added to supports. The activity measurements coupled with the physicochemical characterization data indicated the different catalysts functionality that influences on their reforming activity. Thus, the higher reforming activity for Mg-modified catalyst respect to bare Al{sub 2}O{sub 3} was explained in terms of the lower acidity and better dispersion achieved in the former, while for Ce- and Zr-promoted catalysts the improvement in intrinsic activity was ascribed to the enhancement of water adsorption/dissociation on the Ni-Ce and Ni-Zr interfaces developed on these catalysts. On the other hand, the lower intrinsic activity of La-added catalyst was explained in terms of the dilution effect caused by the presence of lanthanum on Ni surfaces. Characterization of catalysts after reaction showed differences on the amount and type of coke deposited on catalysts surfaces. La and Ce additives were found to prevent the formation of carbon filaments on nickel surfaces, which is responsible of the changes in product selectivities with reaction time observed on Ni/Al{sub 2}O{sub 3}, Ni/ZrO{sub 2}-Al{sub 2}O{sub 3} and Ni/MgO-Al{sub 2}O

  8. Treatment of a non-azo dye aqueous solution by CWAO in continuous reactor using a Ni catalyst derived from hydrotalcite-like precursor

    Energy Technology Data Exchange (ETDEWEB)

    Vallet, Ana, E-mail: avallet@quim.ucm.es [Grupo de Catalisis y Procesos de Separacion (CyPS), Departamento de Ingenieria Quimica, Facultad de Ciencias Quimicas, Universidad Complutense de Madrid, Avda. Complutense s/n, 28040 Madrid (Spain); Besson, Michele, E-mail: michele.besson@ircelyon.univ-lyon1.fr [IRCELYON, Institut de recherches sur la catalyse et l' environnement de Lyon, UMR5256 CNRS-Universite Lyon1, 2 Avenue Albert Einstein, F-69626 Villeurbanne Cedex (France); Ovejero, Gabriel; Garcia, Juan [Grupo de Catalisis y Procesos de Separacion (CyPS), Departamento de Ingenieria Quimica, Facultad de Ciencias Quimicas, Universidad Complutense de Madrid, Avda. Complutense s/n, 28040 Madrid (Spain)

    2012-08-15

    Highlights: Black-Right-Pointing-Pointer Ni supported over hydrotalcite calcined precursors as catalyst. Black-Right-Pointing-Pointer Catalytic wet air oxidation in trickle bed reactor for Basic Yellow 11 removal. Black-Right-Pointing-Pointer Dye removal depends on temperature, initial dye concentration and flow rate. Black-Right-Pointing-Pointer The catalyst proved to be stable and efficient for the dye degradation. - Abstract: Catalytic wet air oxidation (CWAO) of a Basic Yellow 11 (BY11) aqueous solution, chosen as a model of a hardly biodegradable non-azo dye was carried out in a continuous-flow trickle-bed reactor, using nickel supported over hydrotalcite precursor calcined at 550 Degree-Sign C. An increase in the reaction temperature (120-180 Degree-Sign C), and a decrease in dye concentration (1000-3000 ppm) or liquid flow rate (0.1-0.7 mL min{sup -1}) enhanced the CWAO performance in a 30 and 19% for the variation of the temperature and concentration respectively. After a small leaching observed within the first hours, the catalyst proved to be very stable during the 65-day reaction. The CWAO process was found to be very efficient, achieving BY11 conversion up to 95% and TOC conversion up to 85% at 0.1 mL min{sup -1} and 180 Degree-Sign C under 5 MPa air.

  9. Solar H2 evolution in water with modified diketopyrrolopyrrole dyes immobilised on molecular Co and Ni catalyst-TiO2 hybrids.

    Science.gov (United States)

    Warnan, Julien; Willkomm, Janina; Ng, Jamues N; Godin, Robert; Prantl, Sebastian; Durrant, James R; Reisner, Erwin

    2017-04-01

    A series of diketopyrrolopyrrole (DPP) dyes with a terminal phosphonic acid group for attachment to metal oxide surfaces were synthesised and the effect of side chain modification on their properties investigated. The organic photosensitisers feature strong visible light absorption (λ = 400 to 575 nm) and electrochemical and fluorescence studies revealed that the excited state of all dyes provides sufficient driving force for electron injection into the TiO2 conduction band. The performance of the DPP chromophores attached to TiO2 nanoparticles for photocatalytic H2 evolution with co-immobilised molecular Co and Ni catalysts was subsequently studied, resulting in solar fuel generation with a dye-sensitised semiconductor nanoparticle system suspended in water without precious metal components. The performance of the DPP dyes in photocatalysis did not only depend on electronic parameters, but also on properties of the side chain such as polarity, steric hinderance and hydrophobicity as well as the specific experimental conditions and the nature of the sacrificial electron donor. In an aqueous pH 4.5 ascorbic acid solution with a phosphonated DuBois-type Ni catalyst, a DPP-based turnover number (TONDPP) of up to 205 was obtained during UV-free simulated solar light irradiation (100 mW cm-2, AM 1.5G, λ > 420 nm) after 1 day. DPP-sensitised TiO2 nanoparticles were also successfully used in combination with a hydrogenase or platinum instead of the synthetic H2 evolution catalysts and the platinum-based system achieved a TONDPP of up to 2660, which significantly outperforms an analogous system using a phosphonated Ru tris(bipyridine) dye (TONRu = 431). Finally, transient absorption spectroscopy was performed to study interfacial recombination and dye regeneration kinetics revealing that the different performances of the DPP dyes are most likely dictated by the different regeneration efficiencies of the oxidised chromophores.

  10. Influence of Ligand Backbone Structure and Connectivity on the Properties of Phosphine-Sulfonate Pd(II/Ni(II Catalysts

    Directory of Open Access Journals (Sweden)

    Zixia Wu

    2017-05-01

    Full Text Available Phosphine-sulfonate based palladium and nickel catalysts have been extensively studied in ethylene polymerization and copolymerization reactions. Previously, the majority of the research works focused on the modifications of the substituents on the phosphorous atom. In this contribution, we systematically demonstrated that the change of the ligand backbone from benzene to naphthalene could greatly improve the properties of this class of catalysts. In the palladium system, this change could increase catalyst stability and polyethylene molecular weights. In the nickel system, this change could dramatically increase the polyethylene molecular weights. Most interestingly, the change in the connectivity of phosphine and sulfonate moieties to the naphthalene backbone could also significantly influence the catalyst properties.

  11. Hydroconversion of aromatic hydrocarbons with iron sulfates catalysts; Ryusan tetsukei shokubai ni yoru hokozoku kagobutsu no suiso tenkan hanno

    Energy Technology Data Exchange (ETDEWEB)

    Ogata, E.; Horie, K. [The University of Tokyo, Tokyo (Japan). Faculty of Engineering; Saito, I.; Ukegawa, K. [National Institute for Resources and Environment, Tsukuba (Japan); Nishijima, A. [Kochi Prefecture Industrial Technology Center, Kochi (Japan)

    1997-10-30

    In order to develop the suitable catalyst for hydroconversion of coal and heavy materials, possibility of high quality catalyst production from iron sulfates was pursued on the hydroconversion of 1-methylnaphthalene(1-MN) and 4-(1-naphthylmethyl)bibenzyl(NMBB) with iron sulfates in the absence and presence of sulfur(S) at 350degC. Catalystic activity of ferrous sulfate was very low in the absence of S. The activity of ferrous sulfate was dramatically increased with addition of enough S for the hydrogenation of 1-MN and hydrocracking of NMBB. The activity of ferric sulfate, however, did not increase with addition of S. Ferrous sulfate is revealed one of useful catalyst precursors for hydroconversion of heavy aromatic hydrocarbons. 5 refs., 4 tabs.

  12. Preparation and characterization of spinel-type MeFe{sub 2}O{sub 4} (Me = Cu, Cd, Ni and Zn) for catalyst applications

    Energy Technology Data Exchange (ETDEWEB)

    Rezlescu, N., E-mail: reznic@phys-iasi.ro [National Institute of Research and Development for Technical Physics, Iasi Bld. Dimitrie Mangeron 47 (Romania); Rezlescu, E.; Popa, P.D. [National Institute of Research and Development for Technical Physics, Iasi Bld. Dimitrie Mangeron 47 (Romania); Popovici, E. [Al. I. Cuza Unversity, Chemical Faculty, Iasi (Romania); Doroftei, C. [National Institute of Research and Development for Technical Physics, Iasi Bld. Dimitrie Mangeron 47 (Romania); Al. I. Cuza University, Physics Faculty, Iasi (Romania); Ignat, M. [National Institute of Research and Development for Technical Physics, Iasi Bld. Dimitrie Mangeron 47 (Romania); Al. I. Cuza Unversity, Chemical Faculty, Iasi (Romania)

    2013-01-15

    Four kinds of spinel ferrites, MeFe{sub 2}O{sub 4} (Me = Cu, Ni, Zn and Cd), were prepared by so called 'selfcombustion method' using nitrates as precursors. The morphological and structural characterization of the ferrite powders have been performed with various techniques: X-ray diffraction (XRD), to determine the phase composition, SEM observations to evaluate nanostructure characteristics, EDAX spectroscopy to evaluate the chemical composition and BET analysis to determine the specific surface area. The ferrite powders have been tested catalytically in combustion reaction of three diluted gases: acetone/air, ethanol/air and methanol/air. The results revealed a pronounced decrease in the combustion temperature when Cu- and Ni-ferrites are used as catalysts. A probable cause was ascribed to multiple valences of Cu and Ni ions which favor a rapid increase in the oxygen ion species adsorbed on ferrite surface. -- Highlights: Black-Right-Pointing-Pointer A simple and low cost method was used for preparation MeFe{sub 2}O{sub 4} (Me = Cu, Ni, Zn, Cd). Black-Right-Pointing-Pointer XRD and SEM confirm spinel structure and nanosized of crystallites (33-52 nm). Black-Right-Pointing-Pointer The metal-type has a strong influence on the minimum combustion temperature. Black-Right-Pointing-Pointer CuFe{sub 2}O{sub 4} and NiFe{sub 2}O{sub 4} ferrites show superior catalytic activity. Black-Right-Pointing-Pointer The catalytic activity of ferrites is controlled by the O{sub 2} ion vacancies.

  13. Mechanistic aspects of the formation of carbon-nanofibers on the surface of Ni foam: A new microstructured catalyst support

    NARCIS (Netherlands)

    Jarrah, Nabeel A.; van Ommen, J.G.; Lefferts, Leonardus

    2006-01-01

    This paper describes the catalytic formation of a layer of carbon nanofibers (CNFs) on Ni foam, resulting in a new catalytic route for preparing thin, highly macroporous layers. The effect of morphology and surface properties (i.e., grain size and presence of NiO) on the rate formation and

  14. Purification of Sulphate Leach Liquor of Spent Raneynickel Catalyst Containing Al and Ni by Solvent Extraction with Organophosphorus-Based Extractants

    Science.gov (United States)

    Rao, Satunuri Venkateswar; Yang, Dong Hyo; Sohn, Jeong Soo; Kim, Soo-Kyung

    2012-01-01

    Solvent extraction (SX) separation of Al from Ni sulphate leach liquor (LL) of spent Raneynickel catalyst containing 0.12 M Al and 1.448 M Ni using organophosphorus extractants has been investigated. Optimization of process conditions includes aqueous pH, extractant concentration, phase ratio, and stripping. Comparison of Al extraction efficiency with 0.45 M extractant concentration for TOPS 99, PC 88 A, and Cyanex 272 at an equilibrium pH of 2.23 was 81.8%, 98.6%, and 75%, respectively. The corresponding coextraction of Ni was 0.65, 0.6, and 0.9. Among the three extractants screened, PC 88A showed better extraction efficiency for Al at lower pH values than the others. Using 0.45 M PC 88 A, extraction isotherm was obtained at an aqueous-to-organic (A : O) phase ratio of 1 : 1–3 and O : A ratio of 1 : 1–5, which predicted possible separation of Al in 2 stages at A/O ratio of 2. Quantitative stripping was achieved by H2SO4. PMID:22505841

  15. Synthesis of nanostructured NiO/Co3O4 through thermal decomposition of a bimetallic (Ni/Co) metal-organic framework as catalyst for cyclooctene epoxidation

    Science.gov (United States)

    Abbasi, Alireza; Soleimani, Mohammad; Najafi, Mahnaz; Geranmayeh, Shokoofeh

    2017-04-01

    Hydrothermal approach has led to the formation of a three-dimensional metal-organic framework (MOF), [NiCo(μ2-tp)(μ4-tp)(4,4‧-bpy)2]n (1) (tp = terephthalic acid and 4,4‧-bpy = 4,4‧-bipyridine) which was characterized by means of single-crystal X-ray diffraction analysis, powder X-ray diffraction (PXRD), FT-IR spectroscopy, scanning electron microscopy (SEM) and inductive coupled plasma optical emission spectroscopy (ICP-OES). Thermal decomposition of the MOF afforded nanostructured mixed metal oxide, namely NiO/Co3O4. The XRD and SEM analysis confirm the formation of the mixed metal oxide. The nanostructured NiO/Co3O4 demonstrated good catalytic activity and selectivity in the epoxidation of cyclooctene in the presence of tert-butyl hydroperoxide (TBHP) as oxidant.

  16. Bimetal catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ng, K. Y. Simon; Salley, Steve O.; Wang, Huali

    2017-10-03

    A catalyst comprises a carbide or nitride of a metal and a promoter element. The metal is selected from the group consisting of Mo, W, Co, Fe, Rh or Mn, and the promoter element is selected from the group consisting of Ni, Co, Al, Si, S or P, provided that the metal and the promoter element are different. The catalyst also comprises a mesoporous support having a surface area of at least about 170 m.sup.2 g.sup.-1, wherein the carbide or nitride of the metal and the promoter element is supported by the mesoporous support, and is in a non-sulfided form and in an amorphous form.

  17. Co/ZnO and Ni/ZnO catalysts for hydrogen production by bioethanol steam reforming. Influence of ZnO support morphology on the catalytic properties of Co and Ni active phases

    Energy Technology Data Exchange (ETDEWEB)

    Da Costa-Serra, J.F.; Chica, A. [Instituto de Tecnolgia Quimica (UPV-CSIC), Universidad Politecnica de Valencia, Consejo Superior de Investigaciones Cientificas, Avenida de los naranjos s/n, 46022 Valencia (Spain); Guil-Lopez, R. [Instituto de Catalisis y Petroleoquimica, CSIC, Marie Curie 2, Cantoblanco, 28049 Madrid (Spain)

    2010-07-15

    Renewable hydrogen production from steam reforming of bioethanol is an interesting approach to produce sustainable hydrogen. However, simultaneous competitive reactions can occur, decreasing the hydrogen production yield. To overcome this problem, modifications in the steam reforming catalysts are being studied. Ni and Co active phases supported over modified ZnO have been widely studied in hydrogen production from steam reforming of bioethanol. However, the influence of the morphology and particle size of ZnO supports on the catalytic behaviour of the supported Ni and Co has not been reported. In the present work, we show how the morphology, shape, and size of ZnO support particles can control the impregnation process of the metal active centres, which manages the properties of active metallic particles. It has been found that nanorod particles of ZnO, obtained by calcination of Zn acetate, favour the metal-support interactions, decreasing the metallic particle sizes and avoiding metal (Co or Ni) sinterization during the calcination of metal precursors. Small metallic particle sizes lead to high values of active metal exposure surface, increasing the bioethanol conversion and hydrogen production. (author)

  18. Estudo microestrutural do catalisador Ni/gama-Al2O3: efeito da adição de CeO2 na reforma do metano com dióxido de carbono Microstructural study of Ni/gamma-Al2O3 catalyst: addition effects of CeO2 on carbon dioxide reforming of methane

    Directory of Open Access Journals (Sweden)

    Antoninho Valentini

    2003-10-01

    Full Text Available The carbon dioxide reforming of methane was carried out over nickel catalysts supported on the gamma-Al2O3/CeO2 system prepared by wet impregnation. With the increase of the CeO2 weight in the catalyst, a higher stability was observed in the catalytic activity, together with an excellent resistance to carbon deposition and a better Ni dispersion. The catalysts were characterized by means of surface area measurements, TPR, H2 chemisorption, XRD, SEM, EDX, XPS and TEM. An interaction between Ni and CeO2 was observed to the Ni/CeO2 sample after activation in a H2 atmosphere above 300 ºC. Such behavior has a significantly influence on the catalytic activity.

  19. Solar-Driven Reduction of Aqueous Protons Coupled to Selective Alcohol Oxidation with a Carbon Nitride-Molecular Ni Catalyst System.

    Science.gov (United States)

    Kasap, Hatice; Caputo, Christine A; Martindale, Benjamin C M; Godin, Robert; Lau, Vincent Wing-Hei; Lotsch, Bettina V; Durrant, James R; Reisner, Erwin

    2016-07-27

    Solar water-splitting represents an important strategy toward production of the storable and renewable fuel hydrogen. The water oxidation half-reaction typically proceeds with poor efficiency and produces the unprofitable and often damaging product, O2. Herein, we demonstrate an alternative approach and couple solar H2 generation with value-added organic substrate oxidation. Solar irradiation of a cyanamide surface-functionalized melon-type carbon nitride ((NCN)CNx) and a molecular nickel(II) bis(diphosphine) H2-evolution catalyst (NiP) enabled the production of H2 with concomitant selective oxidation of benzylic alcohols to aldehydes in high yield under purely aqueous conditions, at room temperature and ambient pressure. This one-pot system maintained its activity over 24 h, generating products in 1:1 stoichiometry, separated in the gas and solution phases. The (NCN)CNx-NiP system showed an activity of 763 μmol (g CNx)(-1) h(-1) toward H2 and aldehyde production, a Ni-based turnover frequency of 76 h(-1), and an external quantum efficiency of 15% (λ = 360 ± 10 nm). This precious metal-free and nontoxic photocatalytic system displays better performance than an analogous system containing platinum instead of NiP. Transient absorption spectroscopy revealed that the photoactivity of (NCN)CNx is due to efficient substrate oxidation of the material, which outweighs possible charge recombination compared to the nonfunctionalized melon-type carbon nitride. Photoexcited (NCN)CNx in the presence of an organic substrate can accumulate ultralong-lived "trapped electrons", which allow for fuel generation in the dark. The artificial photosynthetic system thereby catalyzes a closed redox cycle showing 100% atom economy and generates two value-added products, a solar chemical, and solar fuel.

  20. Polyphosphoric acid supported on Ni0.5Zn0.5Fe2O4 nanoparticles as a magnetically-recoverable green catalyst for the synthesis of pyranopyrazoles

    Directory of Open Access Journals (Sweden)

    Farid Moeinpour

    2017-05-01

    Full Text Available Polyphosphoric acid supported on silica coated Ni0.5Zn0.5Fe2O4 nanoparticles was found to be magnetically separable, highly efficient, eco-friendly, green and recyclable heterogeneous catalyst. This new catalyst at first was fully characterized by TEM, SEM, FTIR and XRD techniques and then catalytic activity of this catalyst was investigated in the synthesis of 5-cyano-1,4-dihydropyrano[2,3-c]pyrazoles. Also the Ni0.5Zn0.5Fe2O4 magnetic nanoparticle-supported polyphosphoric acid could be reused at least six times without significant loss of activity. It could be recovered easily by applying an external magnet.

  1. 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)

  2. Structural changes in a catalyst based on the intermetallide hydride ZrNiH/sub 2. 8/ on activation

    Energy Technology Data Exchange (ETDEWEB)

    Rudnitskii, L.A.; Soboleva, T.N.; Bondartsova, I.I.; Dubyaga, N.A.; Mazus, E.I.; Lunin, V.V.; Alekseev, A.M.

    1988-01-01

    A combination of thermogravimetric and x-ray diffraction analysis was used to study structural changes in the intermetallic hydride catalyst during its activation. Changes in the thickness of the hydride pellets were assessed by dilatometry. The activation of the hydride included oxidative and reductive stages. The activation process led to profound changes in the phase composition and structure of the hydride.

  3. Hydrodechlorination of dichlorobenzenes and their derivatives over Ni-Mo/C catalyst: kinetic analysis and effect of molecular structure of reactant.

    Science.gov (United States)

    Gryglewicz, Stanisław; Piechocki, Wojciech

    2011-04-01

    The kinetics of the catalytic hydrodechlorination (HDC) process of selected dichlorobenzenes (DCBs), dichlorotoluenes (DCTs) and dichlorodiphenyls (DCDs) was studied in the presence of a sulphided carbon-supported Ni-Mo catalyst. The HDC runs were performed in a magnetic stirred batch reactor in the range of 210-230°C under the hydrogen pressure of 3MPa. The kinetic constants were evaluated and the reaction network was proposed assuming the pseudo-first order kinetics of dechlorination process. The HDC of aromatic dichloroderivatives proceeded via a network of sequential-parallel reactions. At 210°C DCBs, DCTs and DCDs followed mainly the pathway of direct transformation to respective aromatic hydrocarbon. At 230°C, the contribution of sequential dechlorination to monochloroderivative became more predominant. Copyright © 2010 Elsevier Ltd. All rights reserved.

  4. Effects of solvent and catalysts on the hydrogenolysis of alkylnaphthalenes; Alkylnaphthalene no suisoka bunkai ni okeru yobai to shokubai no koka

    Energy Technology Data Exchange (ETDEWEB)

    Futamura, S. [National Institute for Resources and Environment, Tsukuba (Japan)

    1996-10-28

    Catalytic effects of metal and carbon materials, which promote hydrogen transfer from hydrogen donor solvents, are investigated during hydrogenolysis of benzyl-1-methylnaphthalenes (BMN) selected as a hydrogen acceptor. For the isomer distribution of BMN after the reaction, almost the same molecular ratio before the reaction was obtained independent of the presence of catalysts. Selectivity of position during the addition of hydrogen atoms from tetralin was not found. For the reaction of BMN in tetralin, 1-methylnaphthalene and toluene were obtained as products, but the formation of benzylnaphthalene was not found. As for the nuclear hydride of BMN, the trace amount formation was confirmed by gas chromatography. For the hydrogen transfer from tetralin progressed catalytically, it was found that the nuclear of naphthalene can not be hydrogenated easily. This was considered to be due to the obstruction of hydrogen transfer from tetralin by the strong adsorption of BMN on the Ni surface. 1 ref., 1 fig., 2 tabs.

  5. Homogeneous Ni catalysts for H2 Oxidation and Production: An Assessment of Theoretical Methods, from Density Functional Theory to Post Hartree-Fock Correlated Wave-Function Theory

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Shentan; Raugei, Simone; Rousseau, Roger J.; Dupuis, Michel; Bullock, R. Morris

    2010-12-09

    A systematic assessment of theoretical methods applicable to the accurate characterization of catalytic cycles of homogeneous catalysts for H2 oxidation and evolution is reported. For these catalysts, H2 bond breaking or formation involve di-hydrogen, di-hydride, hydride-proton, and di-proton complexes. The key elementary steps have heterolytic character. In the context of Density Functional Theory (DFT) we investigated the use of functionals in the generalized gradient approximation (GGA) as well as hybrid functionals. We compared the results with wavefunction theories based on perturbation theory (MP2 and MP4) and on coupled-cluster expansions (CCSD and CCSD(T)). Our findings suggest that DFT results based on Perdew functionals are in semi-quantitative agreement with the CCSD(T) results, with deviations of a few kcal/mol only. On the other hand, the B3LYP functional is not even in qualitative agreement with CCSD[T]. Surprisingly the MP2 results are found to be extremely poor, a finding that we attribute to the limited treatment in MP2 theory of dynamic electron correlation effects in Ni(0) oxidation state. This material is based upon work supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences.

  6. Correlating Oxygen Evolution Catalysts Activity and Electronic Structure by a High-Throughput Investigation of Ni1-y-zFeyCrzOx

    Science.gov (United States)

    Schwanke, Christoph; Stein, Helge Sören; Xi, Lifei; Sliozberg, Kirill; Schuhmann, Wolfgang; Ludwig, Alfred; Lange, Kathrin M.

    2017-03-01

    High-throughput characterization by soft X-ray absorption spectroscopy (XAS) and electrochemical characterization is used to establish a correlation between electronic structure and catalytic activity of oxygen evolution reaction (OER) catalysts. As a model system a quasi-ternary materials library of Ni1-y-zFeyCrzOx was synthesized by combinatorial reactive magnetron sputtering, characterized by XAS, and an automated scanning droplet cell. The presence of Cr was found to increase the OER activity in the investigated compositional range. The electronic structure of NiII and CrIII remains unchanged over the investigated composition spread. At the Fe L-edge a linear combination of two spectra was observed. These spectra were assigned to FeIII in Oh symmetry and FeIII in Td symmetry. The ratio of FeIII Oh to FeIII Td increases with the amount of Cr and a correlation between the presence of the FeIII Oh and a high OER activity is found.

  7. Zeolite encapsulated Ni(II)-Schiff-base complex: a novel size-selective electro-catalyst for the determination of the purity of stevioside.

    Science.gov (United States)

    Avei, Mehdi Rashvand; Jafarian, Majid; Etezadi, Sedigheh; Gobal, Fereydoon; Khakali, Maryam; Rayati, Saeed; Mahjani, Mohammad Ghasem

    2013-04-15

    Ship-in-a-bottle complex of nickel(II) containing the ligand N,N'-bis(2,4-dihydroxyacetophenone)-2,2-dimethylpropandiimine (H2{salnptn(4-OH)2}) has been synthesized in zeolite Y. The characteristics of the encapsulated complex are identified by the methods of EDX, SEM, XRD, FT-IR and cyclic voltammetry. A catalytic effect in the electrochemical oxidation of glucose, fructose and sucrose, and a blocking effect in stevioside oxidation are demonstrated on the Ni(II){salnptn(4-OH)2}-Y/CPE. The effects of some parameters, such as potential scan rate and concentration of carbohydrates are investigated. The rate constants for the catalytic reaction (k') of carbohydrates are also obtained. The size-selective electro-catalyst shows a good linear dependency on carbohydrates' concentration in the range of 0.01-0.06 M with the detection limit of 6.4mM at the signal-to-noise ratio of 3. Furthermore, the modified electrode exhibits no interference with the simultaneous presence of stevioside. In brief, these results demonstrate that Ni(II){salnptn(4-OH)2}-Y composites have a great potential for synthesizing size-selective electrocatalysts for determining the purity of stevioside. Copyright © 2013 Elsevier B.V. All rights reserved.

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

    Directory of Open Access Journals (Sweden)

    Emma C. Lovell

    2015-03-01

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

  9. Selective Photocatalytic CO2 Reduction in Water through Anchoring of a Molecular Ni Catalyst on CdS Nanocrystals.

    Science.gov (United States)

    Kuehnel, Moritz F; Orchard, Katherine L; Dalle, Kristian E; Reisner, Erwin

    2017-05-31

    Photocatalytic conversion of CO2 into carbonaceous feedstock chemicals is a promising strategy to mitigate greenhouse gas emissions and simultaneously store solar energy in chemical form. Photocatalysts for this transformation are typically based on precious metals and operate in nonaqueous solvents to suppress competing H2 generation. In this work, we demonstrate selective visible-light-driven CO2 reduction in water using a synthetic photocatalyst system that is entirely free of precious metals. We present a series of self-assembled nickel terpyridine complexes as electrocatalysts for the reduction of CO2 to CO in organic media. Immobilization on CdS quantum dots allows these catalysts to be active in purely aqueous solution and photocatalytically reduce CO2 with >90% selectivity under UV-filtered simulated solar light irradiation (AM 1.5G, 100 mW cm-2, λ > 400 nm, pH 6.7, 25 °C). Correlation between catalyst immobilization efficiency and product selectivity shows that anchoring the molecular catalyst on the semiconductor surface is key in controlling the selectivity for CO2 reduction over H2 evolution in aqueous solution.

  10. Synthesis and characterization of bimetallic Pd-Ni catalysts in a CeO{sub 2} matrix for the generation of H{sub 2} by the reforming reaction of methanol; Sintesis y caracterizacion de catalizadores bimetalicos Pd-Ni en una matriz de CeO{sub 2} para la generacion de H{sub 2} mediante la reaccion de reformado de metanol

    Energy Technology Data Exchange (ETDEWEB)

    Contreras C, R.

    2016-07-01

    The hydrothermal method was used for the synthesis of CeO{sub 2} nano rods using Ce(NO{sub 3}){sub 3}·6H{sub 2}O and NH{sub 4}OH. The catalytic support was calcined at 700 degrees Celsius. The synthesis of CeO{sub 2} nano rods were impregnated with an aqueous solution of Ni(NO{sub 3}){sub 2}·6H{sub 2}O by an incipient wetness impregnation method at an appropriate concentration to yield 5 and 15% of Ni in the catalysts. Then 0.5% of Pd was impregnated using PdCl{sub 2}. The samples obtained were calcined at 400 and reduced at 450 degrees Celsius. The catalytic materials were characterized by: temperature programmed reduction (TPR), Scanning Electron Microscopy (Sem) , surface area and X-ray diffraction (XRD) . Sem results showed that the CeO{sub 2} is formed by nano rods and in lesser proportion semi spherical particles. Bet surface area of the catalysts decreases with Ni loading onto the CeO{sub 2} nano rods. Pd O and Ni O were reduced at low and high temperature as was observed by TPR. The CeO{sub 2} one-dimensional nano rods showed a highly crystalline structure with sharp diffraction peaks, with a typical fluorite structure (cubic structure of the CeO{sub 2}) and characteristic peaks corresponding to metallic Ni. No diffraction peaks of Pd were found. This is due to the low concentration of this metal in the catalyst. These catalysts showed high activity and selectivity to H{sub 2} at maximum reaction temperature. According to the results of activity and selectivity, the catalysts with Pd-Ni are an alternative for the H{sub 2} production in auto thermal reforming reaction of methanol. (Author)

  11. Comparative study between traditional and modified Pechini synthesis methods in the preparation of LaNiO{sub 3} and LaNi{sub 0,8}Co{sub 0,2}O{sub 3} catalysts; Estudo comparativo entre os metodos de sintese Pechini tradicional e modificado na confeccao dos catalisadores LaNiO{sub 3} e LaNi{sub 0,8}Co{sub 0,2}O{sub 3}

    Energy Technology Data Exchange (ETDEWEB)

    Silva, F.E.F.; Aquino, F.M.; Silva, M.C.M.F., E-mail: fabio@cear.ufpb.br [Universidade Federal da Paraiba (UFPB), Joao Pessoa, PB (Brazil). Departamento de Engenharia de Energias Renovaveis

    2016-07-01

    One of the ways of obtaining hydrogen is from the methane reforming reaction, which is an endothermic and non-spontaneous reaction. In order to minimize this energy, nickel catalysts are used. This work aims to synthesize and characterize the catalysts LaNiO{sub 3} and LaNi{sub 0,8}Co{sub 0,2}O{sub 3} using the Pechini method, making use of citric acid and ethylene glycol and modified Pechini, using the edible gelatin as a chelating and polymerizing agent. The obtained materials were characterized by X-Ray Diffraction (XRD), where the formation of peaks characteristic of perovskite and monophasic structures was observed. Scanning Electron Microscopy (SEM) showed that porosity and powders with few agglomerates were observed by both methods. In the analysis of determination of the specific surface area (BET) the materials were shown with areas that are according to the literature.

  12. Hierarchical nanostructured NiCo2O4 as an efficient bifunctional non-precious metal catalyst for rechargeable zinc-air batteries

    Science.gov (United States)

    Prabu, Moni; Ketpang, Kriangsak; Shanmugam, Sangaraju

    2014-02-01

    A nickel-doped cobalt oxide spinel structure is a promising non-precious metal electrocatalyst for oxygen evolution and oxygen reduction in rechargeable metal-air batteries and water electrolyzers operating with alkaline electrolytes. One dimensional NiCo2O4 (NCO) nanostructures were prepared by using a simple electrospinning technique with two different metal precursors (metal nitrate/PAN and metal acetylacetonate/PAN). The effect of precursor concentration on the morphologies was investigated. Single-phase, NCO with an average diameter of 100 nm, porous interconnected fibrous morphology was revealed by FESEM and FETEM analysis. The hierarchical nanostructured 1D-spinel NiCo2O4 materials showed a remarkable electrocatalytic activity towards oxygen reduction and evolution in an aqueous alkaline medium. The extraordinary bi-functional catalytic activity towards both ORR and OER was observed by the low over potential (0.84 V), which is better than that of noble metal catalysts [Pt/C (1.16 V), Ru/C (1.01 V) and Ir/C (0.92 V)], making them promising cathode materials for metal-air batteries. Furthermore, the rechargeable zinc-air battery with NCO-A1 as a bifunctional electrocatalyst displays high activity and stability during battery discharge, charge, and cycling processes.A nickel-doped cobalt oxide spinel structure is a promising non-precious metal electrocatalyst for oxygen evolution and oxygen reduction in rechargeable metal-air batteries and water electrolyzers operating with alkaline electrolytes. One dimensional NiCo2O4 (NCO) nanostructures were prepared by using a simple electrospinning technique with two different metal precursors (metal nitrate/PAN and metal acetylacetonate/PAN). The effect of precursor concentration on the morphologies was investigated. Single-phase, NCO with an average diameter of 100 nm, porous interconnected fibrous morphology was revealed by FESEM and FETEM analysis. The hierarchical nanostructured 1D-spinel NiCo2O4 materials showed a

  13. The Synergy Effect of Ni-M (M = Mo, Fe, Co, Mn or Cr Bicomponent Catalysts on Partial Methanation Coupling with Water Gas Shift under Low H2/CO Conditions

    Directory of Open Access Journals (Sweden)

    Xinxin Dong

    2017-02-01

    Full Text Available Ni-M (M = Mo, Fe, Co, Mn or Cr bicomponent catalysts were prepared through the co-impregnation method for upgrading low H2/CO ratio biomass gas into urban gas through partial methanation coupling with water gas shift (WGS. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction (XRD, H2 temperature programmed reduction (H2-TPR, H2 temperature programmed desorption (H2-TPD, scanning electron microscopy (SEM and thermogravimetry (TG. The catalytic performances demonstrated that Mn and Cr were superior to the other three elements due to the increased fraction of reducible NiO particles, promoted dispersion of Ni nanoparticles and enhanced H2 chemisorption ability. The comparative study on Mn and Cr showed that Mn was more suitable due to its smaller carbon deposition rate and wider adaptability to various H2/CO and H2O/CO conditions, indicating its better synergy effect with Ni. A nearly 100 h, the lifetime test and start/stop cycle test further implied that 15Ni-3Mn was stable for industrial application.

  14. Catalisadores sol-gel de Ni-SiO2 e Ni-Al2O3 aplicados na reforma de metano com CO2 = Ni-SiO2 and Ni-Al2O3 sol-gel catalysts applied to methane reforming with CO2

    Directory of Open Access Journals (Sweden)

    Giane Gonçalves

    2005-01-01

    Full Text Available A reação de reforma do metano com CO2 apresenta-se como um processopromissor de geração de gás de síntese e hidrogênio. Neste sentido, foram preparados catalisadores de níquel-sílica e níquel-alumina pelo método sol-gel, com carga metálica nominal de 8% em massa. Os catalisadores foram caracterizados por redução à temperatura programada, análise termogravimétrica e determinação da área superficial específica. A reação de reforma do metano com CO2 foi realizada em um micro-reator contendo 500 mg de catalisador, previamente ativado em uma mistura redutora contendo hidrogênio. Osensaios de reforma a seco do metano foram realizados a 800°C, na pressão atmosférica, por um período de 12 horas, com uma razão molar de alimentação de [CO2:CH4] = 6. Os produtos da reação foram analisados por cromatografia gasosa. Dentre os catalisadoresavaliados, nas condições de reação estudadas, o catalisador de níquel suportado em sílica foi o que apresentou o melhor desempenho.The dry reforming reaction of methane comes as a promising process of syngas and hydrogen. Nickel catalysts on Al2O3 and SiO2 were synthesized by sol-gel method, with metalic load of 8% weight. The catalysts were characterized by temperature programmed reduction (TPR, termogravimetry analysis (TGA and specific surface area measurements (BET. The dry reforming reaction was performed in a micro reactor packed with 500 mg of catalyst, previously activated in atmosphere of hydrogen. The dry reforming tests were done at 800oC and atmospheric pressure by a period of 12 hours, with a molar ratio in the feeding of [CO2:CH4] = 6. The products of the reaction were analyzed by gas chromatograph. The Ni-SiO2 catalysts showed better performance.

  15. In-situ Measurements of the Effect of Au Doping in Ni Catalysts on the Yield of Tubular Carbon Nanostructures

    DEFF Research Database (Denmark)

    Sharma, Renu; Chee, S.; Rez, P.

    During the last five years, in-situ observations using environmental transmission microscopy (ETEM) has played a crucial role in revealing atomic level structural transformations occurring during their nucleation and growth. We have combined in-situ and ex-situ measurements to demonstrate....... Formation of different structures depended upon the rate of growth, which was in turn controlled by pressure and temperature. Both in-situ and ex-situ analysis of the composition of the catalyst particles, effect of temperature and pressure on the morphology and structural mechanism for the formation...... and high resolution were recorded at reaction temperatures and under flowing acetylene to measure growth rates and to follow the growth at atomic resolution. We observed increased activity in tubular structure formation for samples with low amounts of Au (~20% nominal composition). Moreover, tubes...

  16. Effectiveness factors for a commercial steam reforming (Ni) catalyst and for a calcined dolomite used downstream biomass gasifiers

    Energy Technology Data Exchange (ETDEWEB)

    Corella, J.; Narvaez, I.; Orio, A. [Madrid Univ. (Spain). Dept. of Chem. Eng.

    1996-12-31

    A commercial steam reforming catalyst from BASF, the G1-25 S one, and a calcined dolomite, Norte-1, from Cantabria-Spain, have been used, once crushed and sieved to different particle fractions between 1.0 and 4.0 mm. The materials have been tested downstream small pilot biomass gasifiers, bubbling fluidized bed type, gasifying with air and with steam. The Thiele modulus and the effectiveness factor have been calculated at temperatures of 750-850 deg C. It is experimentally shown that diffusion control plays an important part when particle size is larger than ca. 0.5 mm. This has to be taken into account when comparing the quality of the solids for tar elimination. (author) (5 refs.)

  17. 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 CO2 reforming of methane

    KAUST Repository

    Biausque, Gregory

    2015-09-24

    Embodiments of the present disclosure provide for NiPt nanoparticles, compositions and supports including NiPt nanoparticles, methods of making NiPt nanoparticles, methods of supporting NiPt nanoparticles, methods of using NiPt nanoparticles, and the like.

  18. Ni/CeO{sub 2}-Al{sub 2}O{sub 3} catalysts promoted with noble metals for the hydrogen production by ethanol vapor reforming; Catalisadores de Ni/CeO{sub 2}-Al{sub 2}O{sub 3} promovidos com metais nobres para a producao de hidrogenio por reforma a vapor de etanol

    Energy Technology Data Exchange (ETDEWEB)

    Profeti, Luciene P.R.; Ticianelli, Edson Antonio; Assaf, Elisabete Moreira [Universidade de Sao Paulo (IQSC/USP), Sao Carlos, SP (Brazil). Inst. de Quimica]. E-mail: eassaf@iqsc.usp.br

    2008-07-01

    The catalytic activity of Ni/CeO{sub 2}-Al{sub 2}O{sub 3} catalysts modified with noble metals (Ru, Ir, Pt and Pd) was investigated in the steam reforming of ethanol. The catalysts were characterized by energy dispersive spectroscopy, X-ray diffraction, UV-Vis diffuse reflectance spectroscopy and H{sub 2} temperature-programmed reduction-X-ray absorption fine structure (XANES). The results showed that the formation of inactive nickel aluminate was avoided due to the presence of a CeO{sub 2} dispersed on the alumina. The promoting effect of noble metals included a decrease of the reduction temperatures of NiO species interacting with the support due to the hydrogen spillover effect, leading to an increase of the reducibilities of the promoted catalysts The better catalytic performance for the ethanol steam reforming was obtained for the NiPd/CeAl catalyst, which presented an effluent gaseous mixture with the highest H{sub 2} yield. (author)

  19. Thermodynamic Constraints in Using AuM (M = Fe, Co, Ni, and Mo) Alloys as N₂ Dissociation Catalysts: Functionalizing a Plasmon-Active Metal.

    Science.gov (United States)

    Martirez, John Mark P; Carter, Emily A

    2016-02-23

    The Haber-Bosch process for NH3 synthesis is arguably one of the greatest inventions of the 20th century, with a massive footprint in agriculture and, historically, warfare. Current catalysts for this reaction use Fe for N2 activation, conducted at high temperatures and pressures to improve conversion rate and efficiency. A recent finding shows that plasmonic metal nanoparticles can either generate highly reactive electrons and holes or induce resonant surface excitations through plasmonic decay, which catalyze dissociation and redox reactions under mild conditions. It is therefore appealing to consider AuM (M = Fe, Co, Ni, and Mo) alloys to combine the strongly plasmonic nature of Au and the catalytic nature of M metals toward N2 dissociation, which together might facilitate ammonia production. To this end, through density functional theory, we (i) explore the feasibility of forming these surface alloys, (ii) find a pathway that may stabilize/deactivate surface M substituents during fabrication, and (iii) define a complementary route to reactivate them under operational conditions. Finally, we evaluate their reactivity toward N2, as well as their ability to support a pathway for N2 dissociation with a low thermodynamic barrier. We find that AuFe possesses similar appealing qualities, including relative stability with respect to phase separation, reversibility of Fe oxidation and reduction, and reactivity toward N2. While AuMo achieves the best affinity toward N2, its strong propensity toward oxidation could greatly limit its use.

  20. Control of branch formation in ethylene polymerization by a [Ni(h3-2-MeC3H4(diimine] PF6 / DEAC catalyst system

    Directory of Open Access Journals (Sweden)

    Escher Fernanda F. N.

    2001-01-01

    Full Text Available The polymerization of ethylene mediated by [Ni(eta³-2-MeC3H4{ArN=C(HC(H=NAr}] PF6, Ar = 2,6-C6H3iPr2 /DEAC catalyst precursor under mild reaction conditions (reaction temperature between -10 ºC and 25 ºC and ethylene pressure between 109 and 1520 kPa yields high molecular weight branched polyethylene. The degree of branching was modulated by a careful choice of reaction conditions. Thus, at 0 ºC and 109 kPa, the branching degree was 17 branches/1000 backbone carbon atoms and at 25 ºC, it went up to 90 branches/1000 backbone carbon atoms. The nature of the observed branches (methyl, ethyl and longer, their quantity and distribution along the polymer backbone chain can be rationalized in terms of a chain walking process and control of the extend of isomerization by the steric hindrance of the growing chain.

  1. Structure-activity relations for Ni-containing zeolites during NO reduction. II. Role of the chemical state of Ni

    NARCIS (Netherlands)

    Mosqueda Jimenez, B.I.; Jentys, A.; Seshan, Kulathuiyer; Lercher, J.A.

    2003-01-01

    The influence of the metal in Ni-containing zeolites used as catalysts for the reduction of NO with propane and propene was studied. In the fresh catalysts, Ni is located in ion exchange positions for Ni/MOR, Ni/ZSM-5, and Ni/MCM-22. The formation of carbonaceous deposits, the removal of Al from

  2. Catalyst Alloys Processing

    Science.gov (United States)

    Tan, Xincai

    2014-10-01

    Catalysts are one of the key materials used for diamond formation at high pressures. Several such catalyst products have been developed and applied in China and around the world. The catalyst alloy most widely used in China is Ni70Mn25Co5 developed at Changsha Research Institute of Mining and Metallurgy. In this article, detailed techniques for manufacturing such a typical catalyst alloy will be reviewed. The characteristics of the alloy will be described. Detailed processing of the alloy will be presented, including remelting and casting, hot rolling, annealing, surface treatment, cold rolling, blanking, finishing, packaging, and waste treatment. An example use of the catalyst alloy will also be given. Industrial experience shows that for the catalyst alloy products, a vacuum induction remelt furnace can be used for remelting, a metal mold can be used for casting, hot and cold rolling can be used for forming, and acid pickling can be used for metal surface cleaning.

  3. Chlorodiethylaluminum supported on silica: A dinuclear aluminum surface species with bridging μ2-Cl-ligand as a highly efficient co-catalyst for the Ni-catalyzed dimerization of ethene

    KAUST Repository

    Kermagoret, Anthony

    2014-05-01

    Silica-supported chloro alkyl aluminum co-catalysts (DEAC@support) were prepared via Surface Organometallic Chemistry by contacting diethylaluminum chloride (DEAC) and high specific surface silica materials, i.e. SBA-15, MCM-41, and Aerosil SiO2. Such systems efficiently activate NiCl 2(PBu3)2 for catalytic ethene dimerization, with turnover frequency (TOF) reaching up to 498,000 molC2H4/ (molNi h) for DEAC@MCM-41. A detailed analysis of the DEAC@SBA-15 co-catalyst structure by solid-state aluminum-27 NMR at high-field (17.6 T and 20.0 T) and ultrafast spinning rates allows to detect six sites, characterized by a distribution of quadrupolar interaction principal values CQ and isotropic chemical shifts δiso. Identification of the corresponding Al-grafted structures was possible by comparison of the experimental NMR signatures with these calculated by DFT on a wide range of models for the aluminum species (mono- versus di-nuclear, mono- versus bis-grafted with bridging Cl or ethyl). Most of the sites were identified as dinuclear species with retention of the structure of DEAC, namely with the presence of μ2-Cl-ligands between two aluminum, and this probably explains the high catalytic performance of this silica-supported co-catalysts. © 2014 Elsevier Inc. All rights reserved.

  4. Development of the Ni/Al{sub 2}O{sub 3}/ZrO{sub 2} catalyst to steam reforming of the natural gas process; Desenvolvimento do catalisador Ni/Al2O3/ZrO2 para o processo de reforma do gas natural

    Energy Technology Data Exchange (ETDEWEB)

    Neiva, Laedna Souto; Ramalho, Melanea A.F.; Costa, Ana Cristina Figueiredo de Melo; Gama, Lucianna [Universidade Federal de Campina Grande (UFCG), PB (Brazil); Andrade, Heloysa M.C. [Universidade Federal da Bahia (UFBA), Salvador, BA (Brazil); Kiminami, Ruth Herta G.A. [Universidade Federal de Sao Carlos (UFSCAR), SP (Brazil)

    2008-07-01

    The aim of this work is to develop catalyst of the type Ni/{alpha}-Al{sub 2}O{sub 3} modified with 0.005 mol of ZrO{sub 2} and structural, morphologic and catalytic characterizations, aiming employ in the reforming process of the natural gas. The catalytic supports were obtained by synthesis method for combustion reaction according to the concepts of the propellants chemistry. The active species of the catalyst (nickel) was deposited over the support by humid impregnation method. The catalytic supports were characterized by XRD, morphologic analysis by SEM and TEM, textural analysis by BET method before and after of the impregnation with nickel and were done catalytic tests in laboratory. The catalytic supports shows structure without any secondary phase with crystallinity elevated degree and crystal size varying between 5.7 and 7.0 nm. The catalytic test shows that these catalysts promoted a conversion percentile considerable of the natural gas in syngas. (author)

  5. The impact of copper in LaNi{sub 1-x}Cu{sub x}O{sub 3} perovskite-like structures used as catalyst precursors for dry reforming of methane

    Energy Technology Data Exchange (ETDEWEB)

    Vlach, K.; Hoang, D.L.; Armbruster, U.; Martin, A. [Leibniz-Institut fuer Katalyse e.V. an der Universitaet Rostock (Germany)

    2013-11-01

    This work deals with the synthesis of perovskite-like catalyst precursors (LaNi{sub 1-x}Cu{sub x}O{sub 3} with x = 0, 0.2, 0.5, 0.8, 1). These precursors were used to catalyse the dry reforming of methane (DRM) reaction carried out at 973 K, CH{sub 4}/CO{sub 2} = 1 and a GHSV = 18,000 ml/g/h. The precursors were transformed during the course of the reaction to give Ni-Cu/La{sub 2}O{sub 3} solids. We found out that the activity increases with raising Ni content but small Cu admixture suppresses the coke formation substantially. XRD and TEM measurements showed that the transformation led to the formation of small metallic Ni and/or Cu particles. In addition also alloying can be observed. The best catalytic system with respect to activity and suppressed carbon deposition was Ni{sub 0.8}-Cu{sub 0.2}/La{sub 2}O{sub 3} (X{sub CH4} = 61%, X{sub CO2} = 67%). (orig.)

  6. A one-dimensional porous carbon-supported Ni/Mo2C dual catalyst for efficient water splitting† †Electronic supplementary information (ESI) available: Experimental details, XRD patterns, SEM and TEM images, BET and Raman data, and electrochemical tests. See DOI: 10.1039/c6sc03356c Click here for additional data file.

    Science.gov (United States)

    Yu, Zi-You; Duan, Yu; Gao, Min-Rui; Lang, Chao-Chao; Zheng, Ya-Rong

    2017-01-01

    The development of active, stable and low-cost electrocatalysts towards both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) for overall water splitting remains a big challenge. Herein, we report a new porous carbon-supported Ni/Mo2C (Ni/Mo2C-PC) composite catalyst derived by thermal treatment of nickel molybdate nanorods coated with polydopamine, which efficiently and robustly catalyses the HER and OER with striking kinetic metrics in alkaline electrolyte. The catalyst affords low onset potentials of –60 mV for the HER and 270 mV for the OER, as well as small overpotentials of 179 mV for the HER and 368 mV for the OER at a current density of 10 mA cm–2. These results compare favorably to Mo2C-PC, Ni-PC, and most other documented Ni- and Mo-based catalysts. The high activity of Ni/Mo2C-PC is likely due to electron transfer from Ni to Mo2C, leading to a higher Ni valence and a lower Mo valence in the Ni/Mo2C-PC catalyst, as these are HER and OER active species and thus account for the enhanced activity. Remarkably, our home-made alkaline electrolyser, assembled with Ni/Mo2C-PC as a bifunctional catalyst, can enable a water-splitting current density of 10 mA cm–2 to be achieved at a low cell voltage of 1.66 V. PMID:28451234

  7. Hydrogenation of artemisinin to dihydroartemisinin over heterogeneous metal catalysts

    Science.gov (United States)

    Kristiani, Anis; Pertiwi, Ralentri; Adilina, Indri Badria

    2017-01-01

    A series of heterogeneous metal catalysts of Ni, Pd, and Pt, both of synthesized and commercial catalysts were used for hydrogenation of artemisinin to dihydroartemisinin. Their catalytic properties were determsined by Surface Area Analyzer and Thermogravimetry Analyzer. The catalytic properties in various reaction conditions in terms of temperature, pressure, reaction time and reactant/catalyst ratio were also studied. The results catalytic activity tests showed that synthesized catalysts of Ni/zeolite, Ni-Sn/zeolite, Ni/bentonite and Ni-Sn/bentonite were not able to produced dihydroartemisinin and deoxyartemisinin was mainly formed. Meanwhile, commercial catalysts of Ni skeletal, Pd/activated charcoal and Pt/activated charcoal yielded the desired dihydroartemisinin product. Ni skeletal commercial catalyst gave the best performance of hydrogenation artemisinin to dihydroartemisinin in room temperature and low H2 pressure.

  8. Efficient NiII2LnIII2Electrocyclization catalysts for the synthesis oftrans-4,5-diaminocyclopent-2-enones from 2-furaldehyde and primary or secondary amines

    OpenAIRE

    Griffiths, Kieran; Kumar, Prashant; Mattock, James D; Abdul-Sada, Alaa; Pitak, mateusz; Coles, Simon; Navarro, Oscar; Vargas, Alfredo; Kostakis, George E.

    2016-01-01

    A series of heterometallic coordination clusters (CCs) [NiII2LnIII2(L1)4Cl2(CH3CN)2] 2CH3CN [Ln = Y (1Y), Sm (1Sm), Eu (1Eu), Gd (1Gd), or Tb (1Tb)] were synthesized by the reaction of (E)-2-(2-hydroxy-3-methoxybenzylidene-amino)phenol) (H2L1) with NiCl2·6(H2O) and LnCl3·x(H2O) in the presence of Et3N at room temperature. These air-stable CCs can be obtained in very high yields from commercially available materials and are efficient catalysts for the room-temperature domino ring-opening elect...

  9. Homogeneous Ni Catalysts for H2 Oxidation and Production: An Assessment of Theoretical Methods, from Density Functional Theory to Post Hartree-Fock Correlated Wave-Function Theory

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Shentan; Raugei, Simone; Rousseau, Roger; Dupuis, Michel; Bullock, R. Morris

    2010-12-09

    A systematic assessment of theoretical methods applicable to the accurate characterization of catalytic cycles of homogeneous catalysts for H2 oxidation and evolution is reported. The key elementary steps involve heterolytic cleavage of the H-H bond and formation/cleavage of Ni-H and N-H bonds. In the context of density functional theory (DFT), we investigated the use of functionals in the generalized gradient approximation (GGA) as well as hybrid functionals. We compared the results with wave-function theories based on perturbation theory (MP2 and MP4) and on coupled-cluster expansions [CCD, CCSD, and CCSD(T)]. Our findings indicate that DFT results based on Perdew correlation functionals are in semiquantitative agreement with the CCSD(T) results, with deviations of only a few kilocalories/mole. On the other hand, the B3LYP functional is not even in qualitative agreement with CCSD(T). Surprisingly, the MP2 results are found to be extremely poor, in particular for the diproton Ni(0) and dihydride Ni(IV) species on the reaction potential energy surface. The Hartree-Fock reference wave function in MP2 theory gives a poor reference state description for these states that are electron rich on Ni, giving rise to erroneous MP2 energies. Finally, we present a detailed potential-energy diagram for the oxidation of H2 by these catalysts after accounting for the effects of solvation, as modeled by a polarizable continuum, and of free energy estimated at the harmonic level of theory.

  10. Oxidation catalyst

    Science.gov (United States)

    Ceyer, Sylvia T.; Lahr, David L.

    2010-11-09

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

  11. Preparation and characterization of LaNi{sub (1-x)}Co{sub x}O{sub 3} perovskites as catalyst precursors for synthesis gas generation by CO{sub 2} reforming of methane; Sintese e caracterizacao de perovskitas LaNi{sub (1-x)}Co{sub x}O{sub 3} como precursores de catalisadores para a conversao do metano a gas de sintese pela reforma com CO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Lima, Sania Maria de; Assaf, Jose Mansur [Universidade Federal de Sao Carlos, SP (Brazil). Dept. de Engenharia Quimica]. E-mail: psania@iris.ufscar.br

    2007-03-15

    LaNiO{sub 3} perovskite was modified by partial substitution of nickel by cobalt in order to increase the stability and resistance to carbon deposition during the methane CO{sub 2} reforming. The results showed that a suitable combination of precipitation and calcination steps resulted in oxides with the desired structure and with important properties for application in heterogeneous catalysis. The partial substitution of Ni by Co resulted in lower rates of conversion of both the reactants, but the catalyst stability was highly increased. The LaNi{sub 0.3}Co{sub 0.7}O{sub 3} catalyst, calcined at 800 deg C, was the most active under the reaction conditions. (author)

  12. Síntese e caracterização de perovskitas LaNi(1-xCo xO3 como precursores de catalisadores para a conversão do metano a gás de síntese pela reforma com CO2 Preparation and characterization of LaNi(1-xCo xO3 perovskites as catalyst precursors for synthesis gas generation by CO2 reforming of methane

    Directory of Open Access Journals (Sweden)

    Sania Maria de Lima

    2007-04-01

    Full Text Available LaNiO3 perovskite was modified by partial substitution of nickel by cobalt in order to increase the stability and resistance to carbon deposition during the methane CO2 reforming. The results showed that a suitable combination of precipitation and calcination steps resulted in oxides with the desired structure and with important properties for application in heterogeneous catalysis. The partial substitution of Ni by Co resulted in lower rates of conversion of both the reactants, but the catalyst stability was highly increased. The LaNi0.3Co0.7O3 catalyst, calcined at 800 ºC, was the most active under the reaction conditions.

  13. Catalytic applications of keto-stabilised phosphorus ylides based on a macrocyclic scaffold: calixarenes with one or two pendant Ni(P,O)-subunits as ethylene oligomerisation and polymerisation catalysts.

    Science.gov (United States)

    Kuhn, Pierre; Sémeril, David; Jeunesse, Catherine; Matt, Dominique; Lutz, Pierre J; Louis, Rémy; Neuburger, Markus

    2006-08-14

    Four calix[4]arenes containing either one or two ylidic -C(O)CH=PPh3 moieties anchored at p-phenolic carbon atoms were prepared starting from cone-25,27-dipropoxycalix[4]arene (1): 1,3-alternate-5,17-bis(2-triphenylphosphoranylideneacetyl)-25,26,27,28-tetrapropoxycalix[4]arene (12), 1,3-alternate-5-(2-triphenylphosphoranylideneacetyl)-25,26,27,28-tetrapropoxycalix[4]arene (13), cone-5-(2-triphenylphosphoranylideneacetyl)-25,27-dihydroxy-26,28-dipropoxycalix[4]arene (14), cone-5,17-bis(2-triphenylphosphoranylideneacetyl)-25,27-dihydroxy-26,28-dipropoxycalix[4]arene (15). All the ylides were shown to be suitable for the preparation of SHOP-type complexes, i.e. of molecules containing [NiPh{Ph2PCH=C(O)R}(PPh3)] subunits (R = calixarene fragment). The monometallic complexes, namely those obtained from the monophosphorus ylides 13 and 14, proved to be efficient ethylene oligomerisation or polymerisation catalysts. At 80 degrees C, they displayed significantly better activities than the prototype [NiPh{Ph(2)PCH=C(O)Ph}(PPh3)], hence reflecting the beneficial role of the bulky calixarene substituent. The systems derived from the two ylides 12 and 15, both containing two convergent ylidic moieties, resulted in lower activities, the proximity of the two catalytic centres facilitating an intramolecular deactivation pathway during the period of catalyst activation. For the first time, the solid-state structure of a complex containing two "NiPh(P,O)(PPh3)" units as well as that of a SHOP-type complex having two linked phosphorus units were determined.

  14. Performance of polyethylene based radiation grafted anion exchange membrane with polystyrene-b-poly (ethylene/butylene)-b-polystyrene based ionomer using NiCo2O4 catalyst for water electrolysis

    Science.gov (United States)

    Gupta, Gaurav; Scott, Keith; Mamlouk, Mohamed

    2018-01-01

    A soluble anion exchange ionomer with high OH- ion conductivity comparable to that of H+ conductivity of Nafion is synthesised by chloromethylation of polystyrene-b-poly (ethylene/butylene)-b-polystyrene (SEBS) and used with NiCo2O4 electro-catalyst for water electrolysis. The ionomer has an ion exchange capacity of 1.9 mmol g-1 and ionic conductivity of 0.14 S cm-2 at 50 °C. The cell voltage at 20 °C at 100 mA cm-2 is 1.77 and 1.72 V in, 0.1 and 1.0 M NaOH, respectively, for an optimum loading of 10 mg cm-2 NiCo2O4. At 10 mg cm-2 NiCo2O4 electrolyser cell performance is at least equal to or superior to that of IrO2 at 2 mg cm-2 with excellent stability over 1 h. When the catalyst is sprayed on the GDL instead of CCM, the performance is further improved to 1.65 V at 100 mA cm-2 at 60 °C & 0.1 M KOH. The limited AEM electrolyser performance when operating with deionised water in comparison to PEM and alkaline electrolyser arises from the sluggish OER in the AEM environment equivalent to pH of 11.5 and the two orders of magnitude lower HER activity with respect to acid medium combined with the high Tafel slope of 120 mV dec-1.

  15. Characterization of catalysts Rh and Ni/Ce{sub x}Zr{sub 1-x}O{sub 2} for hydrogen production by ethanol steam reforming; Caracterisation de catalyseurs Rhodium et Nickel/ Ce{sub x}Zr{sub 1-x}O{sub 2} pour la production d'hydrogene par vaporeformage de l'ethanol

    Energy Technology Data Exchange (ETDEWEB)

    Birot, A

    2005-07-01

    This work concerned a study on catalytic behaviour of metallic catalysts (Rh or Ni) supported on earth rare oxides Ce{sub x}Zr{sub 1-x}O{sub 2} in ethanol steam reforming in order to produce hydrogen. Catalyst 1%Rh/Ce0,50Zr0,50O{sub 2} showed a good activity with a good hydrogen yield. We turned a study onto understanding inter-conversion reaction between H{sub 2}, CO and CO{sub 2} which lead to CH{sub 4} formation. We also studied intrinsic properties of catalysts. We confirmed basic character of catalysts and a good hydrogenation activity. A good activity in CO hydrogenation allowed to evidence a necessity to use a catalyst which is less active in hydrogenation reaction and with a basic character in order to improve hydrogen yield. (author)

  16. From 3D to 2D Co and Ni Oxyhydroxide Catalysts: Elucidation of the Active Site and Influence of Doping on the Oxygen Evolution Activity

    DEFF Research Database (Denmark)

    Tripkovic, Vladimir; Hansen, Heine Anton; Vegge, Tejs

    2017-01-01

    are ostensibly the most active sites, and Ni ox-hy sheets are more electronically conductive in comparison to their Co equivalents. Furthermore, we examine 25 different doped Co and Ni ox-hy nanosheets (V, Cr, Mn, Fe, Co/Ni, Cu, Ru, Rh, Pd, Ir, Pt, Ag, Al, Ga, In, Sn, Pb, Bi, Mg, Sc, Y, Ti, Nb, Zn, and Cd...... extend the analysis to include bulk terminations and reveal that most dopants, which are stable in the nanosheets, have a large propensity to segregate to the surface of bulk materials, and those that are less prone to segregation (Fe or Cr) are not electronically conductive in the bulk. Overall, we...

  17. Change in catalyst properties during coal liquefaction; Kokoritsu sekitan ekika shokubai no kaihatsu (Hanno no shinko ni tomonau shokubai seijo no henka). 1

    Energy Technology Data Exchange (ETDEWEB)

    Koyama, T.; Sato, K.; Kaneko, T.; Shimasaki, K. [Nippon Brown Coal Liquefaction Co. Ltd., Tokyo (Japan)

    1996-10-28

    The purpose of this study is to prevent the deactivation of catalysts recycled in the 0.1 t/d bench scale unit (BSU). Catalysts recovered during reactions in the BSU and after reactions in the 5-liter autoclave were analyzed, to investigate the influences of the reaction condition on the property and activity of catalysts. Were used {gamma}-iron oxyhydroxide ({gamma}-FeOOH), {alpha}-iron oxyhydroxide ({alpha}-FeOOH), and natural pyrite (FeS2) as catalysts. At the S/Fe atomic ration of 1.2 under the BSU reaction condition, troilite was more easily formed from {gamma}-FeOOH compared with pyrite and {alpha}-FeOOH. As the reaction proceeded through the first, second, and third reactors, the crystal size increased, the pyrrhotite content decreased, and the troilite content increased. Deactivation due to the formation of troilite was irreversible. At the S/Fe of 3.0, however, both the formation of troilite and the crystal growth of pyrrhotite were not observed. It was found that the deactivation of catalysts can be remarkably suppressed. 5 refs., 6 figs., 1 tab.

  18. The capacity of modified nickel catalysts derived from discharged catalyst of fertilizer plants for NOx treatment

    Science.gov (United States)

    Ha, T. M. P.; Luong, N. T.; Le, P. N.

    2016-11-01

    In Vietnam for recent years, a large amount of hazardous waste containing nickel (Ni) derived from discharged catalyst of fertilizer plants has caused environmental problems in landfill overloading and the risk of soil or surface water sources pollution. Taking advantage of discharged catalyst, recycling Ni components and then synthesizing new catalysts apply for mono-nitrogen oxides (NOx) treatments is an approach to bring about both economic and environmental benefits. This study was carried out with the main objective: Evaluate the performance of modified catalysts (using recovered Ni from the discharged RKS-2-7H catalyst of Phu My Fertilizer Plant) on NOx treatment. The catalysts was synthesized and modified with active phases consist of recovered Ni and commercial Barium oxide (BaO), Manganese dioxide (MnO2) / Cerium (IV) oxide (CeO2) on the support Aluminium oxide (γ-Al2O3). The results show that the modified catalysts with Ni, Ba, Ce was not more beneficial for NOx removal than which with Ni, Ba, Mn. 98% NOx removal at 350°C with the start temperature at 115°C and the T60 value at 307°C can be obtained with 10Ni10Ba10Mn/Al catalyst.

  19. Fast microwave-assisted solvothermal synthesis of metal nanoparticles (Pd, Ni, Sn) supported on sulfonated MWCNTs: Pd-based bimetallic catalysts for ethanol oxidation in alkaline medium

    CSIR Research Space (South Africa)

    Ramulifho, T

    2012-01-01

    Full Text Available The preparation of metal nanoparticles (Pd, Ni, Sn) supported on sulfonated multi-walled carbon nanotubes (SF-MWCNTs) using a very rapid microwave-assisted solvothermal strategy has been described. Electrocatalytic behaviour of the SF...

  20. A Study of Deactivating Carbon Species during Methanation on a Ni/Al2O3 Catalyst

    DEFF Research Database (Denmark)

    Olesen, Sine Ellemann

    are prone to deactivate due to sintering and carbon deposition. The latter process is not well understood and thus, this work attempted to further the research in low temperature carbon formation. In order to obtain fundamental knowledge, the experimental setup had to be free of impurities and great care......This Ph.D. thesis describes the research and ndings from experimental testing of a methanation catalyst and the characterisation of said catalyst. Methanation is the conversion of syngas (CO and H2) typically from coal or biomass to methane and water. Methane is the biggest constituent of...

  1. Synthesis NiAl{sub 1,0}Fe{sub 1,0}O{sub 4} catalyst by the combustion reaction to their use in the shift reaction (WGSR); Sintese do catalisador de NiAl{sub 1,0}Fe{sub 1,0}O{sub 4} por reacao de combustao visando sua utilizacao na reacao de shift (WGSR)

    Energy Technology Data Exchange (ETDEWEB)

    Santos, P.T.A.; Costa, A.C.F.M.; Neiva, L.S.; Gama, L. [Universidade Federal de Campina Grande (UFCG), PB (Brazil). Dept. de Engenharia de Materiais; Argolo, F.; Andrade, H.M.C. [Universidade Federal da Bahia (UFBA), Salvador, BA (Brazil). Inst. de Quimica

    2009-07-01

    This work aims at the synthesis of catalyst NiAl{sub 1,0}Fe{sub 1,0}O{sub 4} by combustion reaction using urea as fuel, to evaluate its performance in the production of hydrogen by the reaction of displacement of water vapor (WGSR). The initial composition of the solution was based on valencia total oxidizing and reducing reagents based on the concepts of the chemistry of propellants, using container as a crucible of glassy silica. The resulting powder was characterized by X-ray diffraction, infrared spectroscopy, nitrogen adsorption isotherms (BET), scanning electronic microscope and catalytic tests. The DRX results reveal the presents majoritary phase NiAl{sub 1,0}Fe{sub 1,0}O{sub 4} spinel, the catalyst presents surface area 28 m{sup 2}/g and isotherms type III. Higher conversion CO/CO{sub 2} of 75% CO conversion observed at 500 deg C and catalytic activity of 43 mmolg{sup -1}.h{sup -1} at 450 deg C. (author)

  2. Investigation of the Process Conditions for Hydrogen Production by Steam Reforming of Glycerol over Ni/Al2O3 Catalyst Using Response Surface Methodology (RSM)

    Science.gov (United States)

    Ebshish, Ali; Yaakob, Zahira; Taufiq-Yap, Yun Hin; Bshish, Ahmed

    2014-01-01

    In this work; a response surface methodology (RSM) was implemented to investigate the process variables in a hydrogen production system. The effects of five independent variables; namely the temperature (X1); the flow rate (X2); the catalyst weight (X3); the catalyst loading (X4) and the glycerol-water molar ratio (X5) on the H2 yield (Y1) and the conversion of glycerol to gaseous products (Y2) were explored. Using multiple regression analysis; the experimental results of the H2 yield and the glycerol conversion to gases were fit to quadratic polynomial models. The proposed mathematical models have correlated the dependent factors well within the limits that were being examined. The best values of the process variables were a temperature of approximately 600 °C; a feed flow rate of 0.05 mL/min; a catalyst weight of 0.2 g; a catalyst loading of 20% and a glycerol-water molar ratio of approximately 12; where the H2 yield was predicted to be 57.6% and the conversion of glycerol was predicted to be 75%. To validate the proposed models; statistical analysis using a two-sample t-test was performed; and the results showed that the models could predict the responses satisfactorily within the limits of the variables that were studied. PMID:28788567

  3. Electrochemical behavior of Ni{sub x}W{sub 1-x} materials as catalyst for hydrogen evolution reaction in alkaline media

    Energy Technology Data Exchange (ETDEWEB)

    Oliver-Tolentino, Miguel A. [UPIBI-IPN, Departamento de Ciencias Basicas, Av. Acueducto s/n, Barrio La Laguna, Col. Ticoman, Mexico D.F. 07340 (Mexico); Arce-Estrada, Elsa M. [ESIQIE-IPN Departamento de Ingenieria en Metalurgia y Materiales, UPALM, UPALM, Mexico D.F. 07738 (Mexico); Cortes-Escobedo, Claudia A. [Centro de Investigacion e Innovacion Tecnologica del IPN, Cda. Cecati s/n, Col. Sta. Catarina, CP 02250 Azcapotzalco D.F. (Mexico); Bolarin-Miro, Ana M.; Sanchez-De Jesus, Felix [Area Academica de Ciencias de la Tierra y Materiales, Universidad Autonoma del Estado de Hidalgo, CU, Carr. Pachuca-Tulancingo Km. 4.5, Mineral de la Reforma, CP 42184 Hidalgo (Mexico); Gonzalez-Huerta, Rosa de G. [ESIQIE-IPN, Departamento de Ingenieria Quimica - Laboratorio de Electroquimica y Corrosion, Edif. Z-5 3er piso, UPALM, Mexico D.F. 07738 (Mexico); Manzo-Robledo, Arturo, E-mail: amanzor@ipn.mx [ESIQIE-IPN, Departamento de Ingenieria Quimica - Laboratorio de Electroquimica y Corrosion, Edif. Z-5 3er piso, UPALM, Mexico D.F. 07738 (Mexico)

    2012-09-25

    Highlights: Black-Right-Pointing-Pointer The electrochemical techniques used in this study elucidated the Ni-W surface state. Black-Right-Pointing-Pointer The Ni-W materials were effective for the hydrogen evolution reaction. Black-Right-Pointing-Pointer The prepared alloys exhibited higher catalytic activity than their precursors. Black-Right-Pointing-Pointer The preparation method is relatively simple and effective procedure. - Abstract: In the present work, results of electrochemical evaluation, as well as morphological and structural characterization of Ni{sub x}W{sub 1-x} materials with x = 0.77, 0.64, 0.4, 0.19 and 0.07 processed by means of high energy ball milling from high purity powders are presented. Also, the electrocatalytic performance on the hydrogen evolution reaction (HER) of the Ni{sub x}W{sub 1-x} materials evaluated by linear polarization and cyclic voltammetry techniques in alkaline media at room temperature is discussed. The structural and morphological characterization of the as-prepared materials was carried out using X-ray diffraction (XRD) and scanning electron microscopy (SEM). Results indicated a small-particle clusters and solid solution formation. According to the kinetics parameters the best electrocatalytic activity was observed at Ni{sub 64}W{sub 36}.

  4. Nanoporous PdNi/C electrocatalyst prepared by dealloying high-Ni-content PdNi alloy for formic acid oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Wei; Wang, Hui; Wang, Rongfang [Key Laboratory of Eco-Environment-Related Polymer Materials, Ministry of Education of China, Key Laboratory of Gansu Polymer Materials, College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070 (China); Ji, Shan [South African Institute for Advanced Materials Chemistry, University of the Western Cape, Cape Town 7535 (South Africa)

    2012-12-15

    To improve the electrochemical performance of Pd-based catalysts for formic acid oxidation, a carbon supported nanoporous PdNi catalyst is prepared by dealloying high-Ni-content PdNi alloy nanoparticles in acid solution. The structure of nanoporous PdNi/C catalyst is characterized by X-ray diffraction, transmission electron microscopy and X-ray photoelectron spectroscopy. The electrocatalytic results show that the activity of the nanoporous PdNi/C catalyst is higher than that of nonporous Pd/C catalyst. The results demonstrate that the carbon-supported nanoporous PdNi catalyst has a potential for application in direct formic acid fuel cells. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  5. Novel Anode Catalyst for Direct Methanol Fuel Cells

    OpenAIRE

    Basri, S.; Kamarudin, S. K.; Daud, W. R. W.; Yaakob, Z.; Kadhum, A. A. H.

    2014-01-01

    PtRu catalyst is a promising anodic catalyst for direct methanol fuel cells (DMFCs) but the slow reaction kinetics reduce the performance of DMFCs. Therefore, this study attempts to improve the performance of PtRu catalysts by adding nickel (Ni) and iron (Fe). Multiwalled carbon nanotubes (MWCNTs) are used to increase the active area of the catalyst and to improve the catalyst performance. Electrochemical analysis techniques, such as energy dispersive X-ray spectrometry (EDX), X-ray diffracti...

  6. Co-Pyrolysis Behaviors of the Cotton Straw/PP Mixtures and Catalysis Hydrodeoxygenation of Co-Pyrolysis Products over Ni-Mo/Al2O3 Catalyst

    Directory of Open Access Journals (Sweden)

    Derun Hua

    2015-12-01

    Full Text Available The doping of PP (polypropylene with cotton straw improved the bio-oil yield, which showed there was a synergy in the co-pyrolysis of the cotton straw and PP at the range of 380–480 °C. In a fixed-bed reactor, model compounds and co-pyrolysis products were used for reactants of hydrodeoxygenation (HDO over Ni-Mo/Al2O3. The deoxygenation rate of model compounds decreased over Ni-Mo/Al2O3 in the following order: alcohol > aldehyde > acetic acid > ethyl acetate. The upgraded oil mainly consisted of C11 alkane.

  7. SYNGAS PRODUCTION FROM CO2-REFORMING OF CH4 OVER SOL-GEL SYNTHESIZED Ni-Co/Al2O3-MgO-ZrO2 NANOCATALYST: EFFECT OF ZrO2 PRECURSOR ON CATALYST PROPERTIES AND PERFORMANCE

    Directory of Open Access Journals (Sweden)

    Seyed Mehdi Sajjadi

    2015-05-01

    Full Text Available Ni-Co/Al2O3-MgO-ZrO2 nanocatalyst with utilization of two different zirconia precursors, namely, zirconyl nitrate hydrate (ZNH and zirconyl nitrate solution (ZNS, was synthesized via the sol-gel method. The physiochemical properties of nanocatalysts were characterized by XRD, FESEM, EDX, BET and FTIR analyses and employed for syngas production from CO2-reforming of CH4. XRD patterns, exhibiting proper crystalline structure and homogeneous dispersion of active phase for the nanocatalyst ZNS precursor employed (NCAMZ-ZNS. FESEM and BET results of NCAMZ-ZNS presented more uniform morphology and smaller particle size and consequently higher surface areas. In addition, average particle size of NCAMZ-ZNS was 15.7 nm, which is close to the critical size for Ni-Co catalysts to avoid carbon formation. Moreover, FESEM analysis indicated both prepared samples were nanoscale. EDX analysis confirmed the existence of various elements used and also supported the statements made in the XRD and FESEM analyses regarding dispersion. Based on the excellent physiochemical properties, NCAMZ-ZNS exhibited the best reactant conversion across all of the evaluated temperatures, e.g. CH4 and CO2 conversions were 97.2 and 99% at 850 ºC, respectively. Furthermore, NCAMZ-ZNS demonstrated a stable yield with H2/CO close to unit value during the 1440 min stability test.

  8. Biodiesel production in methyl esterification in the frying oil using catalyst Ni{sub 0,5}Zn{sub 0,5}Fe{sub 2}O{sub 4} to produce biodiesel; Producao de biodiesel por esterificacao metalica utilizando o ferroespinelio Ni{sub 0,5}Zn{sub 0,5}Fe{sub 2}O{sub 4} como catalisador e oleo de fritura como materia prima

    Energy Technology Data Exchange (ETDEWEB)

    Vasconcelos, E.V.; Dantas, J.; Pereira, K.B.O.; Barros, A.B.; Moura, T.F.B.; Costa, A.C.F.M., E-mail: erikvilar12@gmail.com [Universidade Federal de campina Grande, PB (Brazil)

    2016-07-01

    The use of magnetic catalysts for biodiesel production has gaining prominence because of possibility about its recovery and its reuse, as well as, the reuse of materials that would be discarded in the environment. Thus, we propose to evaluate the efficiency of the catalyst Ni{sub 0,5}Zn{sub 0,5}Fe{sub 2}O{sub 4} in methyl esterification in the frying oil to produce biodiesel. The catalyst was produced by combustion reaction using containers with different production capacity and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and infrared spectrometry with Fourier transform (FTIR). The catalytic tests were conducted in a stainless steel reactor at 180°C/1h, 2% of catalyst, oil/ethanol ratio of 1:12. Regardless of the container production capacity it was verified the catalyst obtaining with the major phase formation of the inverse spinel and traces of segregated phases with an average crystallite size of 42.13, 32.07 and 36.93 nm. All catalysts showed satisfactory results with conversions of 74%, 77% and 71%. (author)

  9. Effects of thermal treatment and fluoride ion doping on surface and catalytic properties of NiO–ZrO2 catalysts

    Directory of Open Access Journals (Sweden)

    Abdel Fattah Reham M.

    2016-03-01

    Full Text Available ZrO2 and a series of NiO/ZrO2 hydrogels (5 to 25 wt.% NiO were co-precipitated with the aid of NaOH–Na2C2O4 solution. Two fluorinated hydrogels were also prepared by wet impregnation method. The samples were calcined in the temperature range of 550 to 850 °C. The surface properties of the samples were determined using DTA, XRD and nitrogen adsorption at −196 °C. The conversion of isopropanol was tested using microcatalytic pulse technique. DTA measurements showed that the addition of nickel oxide to zirconia influences the phase transition of ZrO2. XRD revealed that the tetragonal phase was formed at T ⩽ 650 °C, while a biphasic mixture was obtained at T ⩾ 750 °C. No spinel structure was detected by both DTA and XRD techniques and only traces of cubic NiO were detected for the samples containing ⩾ 15 wt.% nickel oxide and calcined at T ⩾ 750 °C. Significant changes in texture, surface acidity and catalytic activity were found as a result of the effects of thermal treatment and chemical composition. Incorporation of fluoride ions greatly increased the surface acidity and consequently enhanced the dehydration activity. It has been found that dehydration activity is related to the amount of surface acidity while the dehydrogenation of this alcohol is sensitive to NiO content.

  10. Molecular characterization of organically bound sulphur in crude oils. A feasibility study for the application of Raney Ni desulphurization as a new method to characterize crude oils

    NARCIS (Netherlands)

    Sinninghe Damsté, J.S.; Rijpstra, W.I.C.; Leeuw, J.W. de; Lijmbach, G.W.M.

    1994-01-01

    Five crude oils with varying sulfur contents (0.1 – 4.7%) were characterized on a molecular level for organically-bound sulfur. Aromatic fractions were analyzed by GC-(MS) and asphaltene and polar fractions were analyzed by flash pyrolysis-GC-(MS). The polar fractions were also desulfurized with

  11. HYDROGENATION OF TOLUENE ON Ni-Co-Mo SUPPORTED ...

    African Journals Online (AJOL)

    HOD

    a bimetallic catalyst system; zeolite-alumina composite supported NiMo catalyst was developed and used in ..... the XRD patterns of molybdenum oxide supported over mesoporous alumina with small crystal sizes ranging ..... oil hydrocracking catalysts using amorphous silica-alumina and zeolites as catalysts supports,".

  12. Steady state performance of copper impregnated Ni/PTFE gas diffusion electrode in alkaline fuel cell

    Energy Technology Data Exchange (ETDEWEB)

    Al-Saleh, M.A.; Gultekin, S.; Al-Zakri, A.S.; Khan, A.A.A. [King Fahd Univ. of Petroleum and Minerals, Dhahran (Saudi Arabia). Dept. of Chemical Engineering

    1996-12-31

    The steady-state polarization measurements on a Raney nickel gas diffusion electrode impregnated with copper oxide were carried out in a half-cell setup with 25% KOH electrolyte solution. Pure hydrogen gas was used at a pressure of 1.2 bars in the temperature range of 25-75{sup o}C. The results were compared with almost the same electrode without copper. There was an improvement in the performance of the electrode impregnated with about 8 wt% Cu. This improvement is much more pronounced at higher temperatures and higher current densities. The spherical Raney catalyst grain model was used to determine the kinetic parameters such as exchange current density (i{sub o}) and charge transfer coefficient ({alpha}) for the electrode. The values found for the exchange current densities at various temperatures were 6.6 x 10{sup -6} -3.1 x 10{sup -4} mA cm{sup -2} and for the charge transfer coefficient was about 0.6. The exchange current density followed an exponential relation with temperature. The apparent activation energy for the electrode reaction at zero mV overvoltage was found to be lower (28 kJ mol{sup -1}) than that reported in the literature (32 kJ mol{sup -1}). The higher values for the exchange current densities and lower values for the activation energies are indication of better performance of the electrode used in this study. (Author)

  13. La-Sr-Ni-Co-O based perovskite-type solid solutions as catalyst precursors in the CO{sub 2} reforming of methane

    Energy Technology Data Exchange (ETDEWEB)

    Valderrama, Gustavo [Laboratorio de Catalisis, Petroleo y Petroquimica, Unidad de Estudios Basicos, Universidad de Oriente - Nucleo Bolivar, La Sabanita - Calle San Simon, Estado Bolivar 8001 (Venezuela); Kiennemann, Alain [Laboratoire des Materiaux et Procedes pour la Catalyse, UMR 7515, ECPM, Universite Louis Pasteur, 25 rue Becquerel, 67087 Strasbourg Cedex 2 (France); Goldwasser, Mireya R. [Centro de Catalisis, Petroleo y Petroquimica, Facultad de Ciencias - Universidad Central de Venezuela. Paseo los Ilustres, Los Chaguaramos, Caracas 1040 (Venezuela)

    2010-04-02

    La{sub 1-x}Sr{sub x}Ni{sub 0.4}Co{sub 0.6}O{sub 3} and La{sub 0.8}Sr{sub 0.2}Ni{sub 1-y}Co{sub y}O{sub 3} solid solutions with perovskite-type structure were synthesized by the sol-gel resin method and used as catalytic precursors in the dry reforming of methane with CO{sub 2} to syngas, between 873 and 1073 K at atmospheric pressure under continuous flow of reactant gases with CH{sub 4}/CO{sub 2} = 1 ratio. These quaternary oxides were characterized by X-ray diffraction (XRD), BET specific surface area and temperature-programmed reduction (TPR) techniques. XRD analyses of the more intense diffraction peaks and cell parameter measurements showed formation of La-Sr-Ni-Co-O solid solutions with La{sub 0.9}Sr{sub 0.1}CoO{sub 3} and/or La{sub 0.9}Sr{sub 0.1}NiO{sub 3} as the main crystallographic phases present on the solids depending on the degree of substitution. TPR analyses showed that Sr doping decreases the temperature of reduction via formation of intermediary species producing Ni{sup 0}, Co{sup 0} with particle sizes in the range of nanometers over the SrO and La{sub 2}O{sub 3} phases. These metallic nano particles highly dispersed in the solid matrix are responsible for the high activity shown during the reaction and avoid carbon formation. The presence of Sr in doping quantities also promotes the secondary reactions of carbon formation and water-gas shift in a very small extension during the dry reforming reaction. (author)

  14. The promotional role of Ni in FeVO4/TiO2 monolith catalyst for selective catalytic reduction of NOx with NH3

    Science.gov (United States)

    Wu, Ganxue; Feng, Xi; Zhang, Hailong; Zhang, Yanhua; Wang, Jianli; Chen, Yaoqiang; Dan, Yi

    2018-01-01

    The promotional effect of nickel additive on the catalytic performance of the representative FeVO4/TiO2 for NH3-SCR reaction is systematically studied for the first time in the present work. The experimental results showed that NOx conversion at low temperature and N2 selectivity could be significantly improved by Ni doping and 0.4Ni-FeV-Ti exhibited the highest NOx removal efficiency. Analysis by XRD, SEM/HR-TEM, Raman, TPD, DRIFTS, TPR and XPS showed that nickel doping effectively promoted the interaction of FeVO4 nanoparticles with TiO2, consequently resulting in an enhanced acidity property, improved redox activity and giving rise to the formation of the surface oxygen vacancies and defect sites.

  15. Novel Fe3O4@SiO2@Ag@Ni trepang-like nanocomposites: High-efficiency and magnetic recyclable catalysts for organic dye degradation

    Science.gov (United States)

    Li, Chao; Sun, Jun-Jie; Chen, Duo; Han, Guang-Bing; Yu, Shu-Yun; Kang, Shi-Shou; Mei, Liang-Mo

    2016-08-01

    A facile step-by-step approach is developed for synthesizing the high-efficiency and magnetic recyclable Fe3O4@SiO2@Ag@Ni trepang-like nanocomposites. This method involves coating Fe2O3 nanorods with a uniform silica layer, reduction in 10% H2/Ar atmosphere to transform the Fe2O3 into magnetic Fe3O4, and finally depositing Ag@Ni core-shell nanoparticles on the L-lysine modified surface of Fe3O4@SiO2 nanorods. The fabricated nanocomposites are further characterized by x-ray diffraction, transmission electron microscopy, scanning electron microscope, Fourier transform infrared spectroscopy, and inductively coupled plasma mass spectroscopy. The Fe3O4@SiO2@Ag@Ni trepang-like nanocomposites exhibit remarkably higher catalytic efficiency than monometallic Fe3O4@SiO2@Ag nanocomposites toward the degradation of Rhodamine B (RhB) at room temperature, and maintain superior catalytic activity even after six cycles. In addition, these samples could be easily separated from the catalytic system by an external magnet and reused, which shows great potential applications in treating waste water. Project supported by the National Basic Research Program of China (Grant No. 2015CB921502), the National Natural Science Foundation of China (Grant Nos. 11474184 and 11174183), the 111 Project (Grant No. B13029), and the Fundamental Research Funds of Shandong University, China.

  16. Dynamical properties of nano-structured catalysts for methane conversion: an in situ scattering study

    DEFF Research Database (Denmark)

    Kehres, Jan

    range from 298 - 1023 K. Correlated crystallite and particle growth due to sintering were observed after the decomposition of the surfactant. Furthermore transformations from rod to spherical particle shape were observed. In situ reduction experiments of a Ni/MgAl2O4 catalyst were performed. The Ni......The reactivity of catalyst particles can be radically enhanced by decreasing their size down to the nanometer range. The nanostructure of a catalyst can have an enormous and positive influence on the reaction rate, for example strong structure sensitivity was observed for methane reforming....../NiO particles in a fresh catalyst sample showed a Ni/NiO core shell structure. The Ni lattice parameter decreased during the reduction due to the release of stress between the Ni core and the NiO shell. Ni particles sintered during heating in hydrogen after the reduction of the NiO shell. Dry reforming...

  17. A high-throughput study of the redox properties of Nb-Ni oxide catalysts by low temperature CO oxidation: Implications in ethane ODH

    KAUST Repository

    Laveille, Paco

    2013-03-01

    CO oxidation is used as a probe reaction to evaluate the redox properties of catalysts for the low temperature oxidative dehydrogenation (ODH) of ethane. Three series of Nb1-x-NixO nanocomposites with various Nb contents (x = 1, 0.95, 0.90, 0.85, 0.80) are prepared by a sol-gel route based on citrate and tested in a 16 parallel fixed-bed unit. Reductive and oxidative pre-treatments are shown to influence both the activity and the stability of the catalysts in CO oxidation. The extent of this effect depends on the Nb content of the composites, the Nb-rich samples being generally the most affected. However, the order of reactivity in CO oxidation is the same for the three series and is maintained whatever the conditions of the pre-treatment. It is the same as that observed in Nb1-x-NixO-catalyzed ethane ODH. © 2012 Elsevier B.V. All rights reserved.

  18. Sintering of nickel steam reforming catalysts

    DEFF Research Database (Denmark)

    Sehested, Jens; Larsen, Niels Wessel; Falsig, Hanne

    2014-01-01

    . In this paper, particle migration and coalescence in nickel steam reforming catalysts is studied. Density functional theory calculations indicate that Ni-OH dominate nickel transport at nickel surfaces in the presence of steam and hydrogen as Ni-OH has the lowest combined energies of formation and diffusion...

  19. Trends in activity for the water electrolyser reactions on 3d M(Ni,Co,Fe,Mn) hydr(oxy)oxide catalysts.

    Science.gov (United States)

    Subbaraman, Ram; Tripkovic, Dusan; Chang, Kee-Chul; Strmcnik, Dusan; Paulikas, Arvydas P; Hirunsit, Pussana; Chan, Maria; Greeley, Jeff; Stamenkovic, Vojislav; Markovic, Nenad M

    2012-05-06

    Design and synthesis of materials for efficient electrochemical transformation of water to molecular hydrogen and of hydroxyl ions to oxygen in alkaline environments is of paramount importance in reducing energy losses in water-alkali electrolysers. Here, using 3d-M hydr(oxy)oxides, with distinct stoichiometries and morphologies in the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) regions, we establish the overall catalytic activities for these reaction as a function of a more fundamental property, a descriptor, OH-M(2+δ) bond strength (0 ≤ δ ≤ 1.5). This relationship exhibits trends in reactivity (Mn < Fe < Co < Ni), which is governed by the strength of the OH-M(2+δ) energetic (Ni < Co < Fe < Mn). These trends are found to be independent of the source of the OH, either the supporting electrolyte (for the OER) or the water dissociation product (for the HER). The successful identification of these electrocatalytic trends provides the foundation for rational design of 'active sites' for practical alkaline HER and OER electrocatalysts.

  20. Catalytic activities of Co(Ni)Mo/TiO{sub 2}-Al{sub 2}O{sub 3} catalysts in gasoil and thiophene HDS and pyridine HDN: effect of the TiO{sub 2}-Al{sub 2}O{sub 3} composition

    Energy Technology Data Exchange (ETDEWEB)

    Borque, M.P.; Lopez-Agudo, A. [Instituto de Catalisis y Petroleoquimica, CSIC, Cantoblanco, 28049 Madrid (Spain); Olguin, E.; Vrinat, M. [Institut de Recherches sur la Catalyse, 2 avenue Albert Einstein, 69626 Villeurbanne Cedex (France); Cedeno, L.; Ramirez, J. [Unicat, Facultad de Quimica UNAM, Cd. Universitaria, 04510 Mexico DF (Mexico)

    1999-04-19

    The effect of the TiO{sub 2}-Al{sub 2}O{sub 3} mixed oxide support composition on the hydrodesulfurization (HDS) of gasoil and the simultaneous HDS and hydrodenitrogenation (HDN) of gasoil+pyridine was studied over two series of CoMo and NiMo catalysts. The intrinsic activities for gasoil HDS and pyridine HDN were significantly increased by increasing the amount of TiO{sub 2} into the support, and particularly over rich- and pure-TiO{sub 2}-based catalysts. It is suggested that the increase in activity be due to an improvement in reducing and sulfiding of molybdena over TiO{sub 2}. The inhibiting effect of pyridine on gasoil HDS was found to be similar for all the catalysts, i.e., was independent of the support composition. The ranking of the catalysts for the gasoil HDS test differed from that obtained for the thiophene test at different hydrogen pressures. In the case of gasoil HDS, the activity increases with TiO{sub 2} content and large differences are observed between the catalysts supported on pure Al{sub 2}O{sub 3} and pure TiO{sub 2}. In contrast, in the case of the thiophene test, the pure Al{sub 2}O{sub 3}-based catalyst appeared relatively more active than the catalysts supported on mixed oxides. Also, in the thiophene test the difference in intrinsic activity between the pure Al{sub 2}O{sub 3}-based catalyst appeared relatively more active than the catalysts supported on mixed oxides. Also in the thiophene test, the difference in intrinsic activity between the pure Al{sub 2}O{sub 3}- and pure TiO{sub 2}-based catalysts is relatively small and dependent on the H{sub 2} pressure used. Such differences in activity trend among the gasoil and the thiophene tests are due to a different sensitivity of the catalysts (by different support or promoter) to the experimental conditions used. The results of the effect of the H{sub 2} partial pressure on the thiophene HDS, and on the effect of H{sub 2}S concentration on gasoil HDS demonstrate the importance of these

  1. Ring Opening of Naphthenic Molecules Over Metal Containing Mesoporous Y Zeolite Catalyst.

    Science.gov (United States)

    Lee, You-Jin; Kim, Eun Sang; Kim, Tae-Wan; Kim, Chul-Ung; Jeong, Kwang-Eun; Lee, Chang-Ha; Jeong, Soon-Yong

    2015-07-01

    Mesoporous Y zeolite (Meso-Y) with a uniform mesopore was synthesized via pseudomorphic syn- thesis. The Meso-Y supported Ni-W catalyst (NiW/Meso-Y) was introduced as a catalyst for the selective ring opening of naphthenic rings. The catalytic test for the ring opening of naphthalene as a model compound of multi-ring aromatics was performed using a batch-type reaction system with both sulfided 20 wt% NiW/Meso-Y and NiW/Y catalysts under different reaction conditions. The catalytic results reveal that the Meso-Y supported NiW catalyst experiences a naphthalene conversion similar to the NiW/Y catalyst, but the NiW/Meso-Y catalyst has higher product yields for BTEX (benzene, toluene, ethyl benzene, and xylene) and the middle distillate than those of the NiW/Y catalyst at a low reaction temperature. These results suggest that the mesoporosity of the NiW/Meso-Y catalyst is more advantageous for the ring opening reaction of multi-ring aromatics due to the easier access for the bulky molecules compared to the NiW/Y catalyst.

  2. Development of active, and stable water-gas-shift reaction catalysts for fuel cell applications

    NARCIS (Netherlands)

    Azzam, K.G.H.; Babich, Igor V.; Seshan, Kulathu Iyer; Lefferts, Leon

    2006-01-01

    Water-gas-shift (WGS) reaction CO + H2O = CO2 + H2, is a key step in the generation of H2 for fuel cells. Noble metal-based catalysts are promising single stage WGS catalysts because they less sensitive than LTS catalysts (Cu based) and more active than the HTS (Ni) catalysts. High activity in CO

  3. 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.

  4. Novel Reforming Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Pfefferle, Lisa D; Haller, Gary L

    2012-10-16

    Aqueous phase reforming is useful for processing oxygenated hydrocarbons to hydrogen and other more useful products. Current processing is hampered by the fact that oxide based catalysts are not stable under high temperature hydrothermal conditions. Silica in the form of structured MCM-41 is thermally a more stable support for Co and Ni than conventional high surface area amorphous silica but hydrothermal stability is not demonstrated. Carbon nanotube supports, in contrast, are highly stable under hydrothermal reaction conditions. In this project we show that carbon nanotubes are stable high activity/selectivity supports for the conversion of ethylene glycol to hydrogen.

  5. Vapor phase hydrogenation of furfural over nickel mixed metal oxide catalysts derived from layered double hydroxides

    Energy Technology Data Exchange (ETDEWEB)

    Sulmonetti, Taylor P.; Pang, Simon H.; Claure, Micaela Taborga; Lee, Sungsik; Cullen, David A.; Agrawal, Pradeep K.; Jones, Christopher W.

    2016-05-01

    The hydrogenation of furfural is investigated over various reduced nickel mixed metal oxides derived from layered double hydroxides (LDHs) containing Ni-Mg-Al and Ni-Co-Al. Upon reduction, relatively large Ni(0) domains develop in the Ni-Mg-Al catalysts, whereas in the Ni-Co-Al catalysts smaller metal particles of Ni(0) and Co(0), potentially as alloys, are formed, as evidenced by XAS, XPS, STEM and EELS. All the reduced Ni catalysts display similar selectivities towards major hydrogenation products (furfuryl alcohol and tetrahydrofurfuryl alcohol), though the side products varied with the catalyst composition. The 1.1Ni-0.8Co-Al catalyst showed the greatest activity per titrated site when compared to the other catalysts, with promising activity compared to related catalysts in the literature. The use of base metal catalysts for hydrogenation of furanic compounds may be a promising alternative to the well-studied precious metal catalysts for making biomass-derived chemicals if catalyst selectivity can be improved in future work by alloying or tuning metal-oxide support interactions.

  6. Stable hydrogen production from ethanol through steam reforming reaction over nickel-containing smectite-derived catalyst.

    Science.gov (United States)

    Yoshida, Hiroshi; Yamaoka, Ryohei; Arai, Masahiko

    2014-12-25

    Hydrogen production through steam reforming of ethanol was investigated with conventional supported nickel catalysts and a Ni-containing smectite-derived catalyst. The former is initially active, but significant catalyst deactivation occurs during the reaction due to carbon deposition. Side reactions of the decomposition of CO and CH4 are the main reason for the catalyst deactivation, and these reactions can relatively be suppressed by the use of the Ni-containing smectite. The Ni-containing smectite-derived catalyst contains, after H2 reduction, stable and active Ni nanocrystallites, and as a result, it shows a stable and high catalytic performance for the steam reforming of ethanol, producing H2.

  7. Hybrid NiCoOx adjacent to Pd nanoparticles as a synergistic electrocatalyst for ethanol oxidation

    Science.gov (United States)

    Wang, Wei; Yang, Yan; Liu, Yanqin; Zhang, Zhe; Dong, Wenkui; Lei, Ziqiang

    2015-01-01

    To improve the electrocatalytic activity of Pd for ethanol oxidation, hybrid NiCoOx adjacent to Pd catalyst (Pd-NiCoOx/C) is successfully synthesized. Physical characterization shows NiCoOx is closely adjacent to Pd nanoparticles in Pd-NiCoOx/C catalyst, which leads to Strong Metal-Support Interactions (SMSI) between the NiCoOx and Pd nanoparticles, in favor of the electrocatalytic properties. The Pd-NiCoOx/C catalyst is estimated to own larger electrochemically active surface area than Pd/C and Pd-NiO/C catalysts. Moreover, compared to Pd/C catalyst, the onset potential of Pd-NiCoOx/C catalyst is negative 40 mV for ethanol oxidation. Noticeably, the current density of Pd-NiCoOx/C catalyst is 2.05 and 1.43 times higher contrasted to Pd/C and Pd-NiO/C catalysts accordingly. Importantly, the Pd-NiCoOx/C catalyst exhibits better stability during ethanol oxidation, which is a promising electrocatalyst for application in direct alkaline alcohol fuel cells.

  8. Catalysts development to base of Cu and Ni supported in ZrO{sub 2} for the H{sub 2} generation by the methanol reformed in oxidizing atmosphere;Desarrollo de catalizadores a base de Cu y Ni soportados en ZrO{sub 2} para la generacion de H{sub 2} mediante el reformado de metanol en atmosfera oxidante

    Energy Technology Data Exchange (ETDEWEB)

    Lopez C, P.; Gutierrez, A.; Gutierrez W, C.; Mendoza A, D.; Martinez, G.; Perez H, R., E-mail: raul.perez@inin.gob.m [ININ, Departamento de Tecnologia de Materiales, Carretera Mexico-Toluca s/n, Ocoyoacac 52750, Estado de Mexico (Mexico)

    2009-07-01

    The search of new alternating sources of energy is at the present time one of the primordial objectives to world level because of the global heating caused by the high emissions of CO{sub 2} at the atmosphere. In this sense the employment of H{sub 2} through the fuel cells offers a more viable alternative for the use of the energy coming from the connection H-H that can be appointed for use of mobile, industrial and homemade applications. However, to generate H{sub 2} in enough quantities is a great challenge at technological level for the necessity of to count with highly selective and efficient catalysts to low reaction temperatures as well as a source that comes from renewable resources. Under this context the methanol reformed in oxidizing atmosphere offers great ecological as energetics and industrial advantages; inside this investigation plane, the Cu seems to be one of the suitable candidates for this reaction due to its high capacity to generate H{sub 2}, besides the great potential of improvement in its physical-chemical properties when being worked in nano metric size and /or associated with other materials. On the other hand, it is known that the Ni addition improvement the catalytic properties because of a better material dispersion, what offers big possibilities of being applied in the H{sub 2} generation in situ by means of the methanol reformed reaction in oxidizing atmosphere; and that the conformation of bimetallic particles Cu/Ni presented high selectivity and catalytic activity for the reaction in question. (Author)

  9. Synthesis and catalytic performance of SiO2@Ni and hollow Ni microspheres

    Science.gov (United States)

    Liu, Xin; Liu, Yanhua; Shi, Xueting; Yu, Zhengyang; Feng, Libang

    2016-11-01

    Nickel (Ni) catalyst has been widely used in catalytic reducing reactions such as catalytic hydrogenation of organic compounds and catalytic reduction of organic dyes. However, the catalytic efficiency of pure Ni is low. In order to improve the catalytic performance, Ni nanoparticle-loaded microspheres can be developed. In this study, we have prepared Ni nanoparticle-loaded microspheres (SiO2@Ni) and hollow Ni microspheres using two-step method. SiO2@Ni microspheres with raspberry-like morphology and core-shell structure are synthesized successfully using SiO2 microsphere as a template and Ni2+ ions are adsorbed onto SiO2 surfaces via electrostatic interaction and then reduced and deposited on surfaces of SiO2 microspheres. Next, the SiO2 cores are removed by NaOH etching and the hollow Ni microspheres are prepared. The NaOH etching time does no have much influence on the crystal structure, shape, and surface morphology of SiO2@Ni; however, it can change the phase composition evidently. The hollow Ni microspheres are obtained when the NaOH etching time reaches 10 h and above. The as-synthesized SiO2@Ni microspheres exhibit much higher catalytic performance than the hollow Ni microspheres and pure Ni nanoparticles in the catalytic reduction of methylene blue. Meanwhile, the SiO2@Ni catalyst has high stability and hence it can be recycled for reuse.

  10. The Effect of Catalyst Support on the Decomposition of Methane to Hydrogen and Carbon

    Directory of Open Access Journals (Sweden)

    Sharif Hussein Sharif Zein Abdul Rahman Mohamed

    2012-10-01

    Full Text Available Decomposition of methane into carbon and hydrogen over Cu/Ni supported catalysts was investigated. The catalytic activities and the lifetimes of the catalysts were studied. Cu/Ni supported on TiO2 showed high activity and long lifetime for the reaction. Transmission electron microscopy (TEM studies revealed the relationship between the catalyst activity and the formation of the filamentous carbon over the catalyst after methane decomposition. While different types of filamentous carbon formed on the various Cu/Ni supported catalysts, an attractive carbon nanotubes was observed in the Cu/Ni supported on TiO2. Key Words:  Methane decomposition, carbon nanotube, Cu/Ni supported catalysts.

  11. Catalyst mixtures

    Science.gov (United States)

    Masel, Richard I.; Rosen, Brian A.

    2017-02-14

    Catalysts that include at least one catalytically active element and one helper catalyst can be used to increase the rate or lower the overpotential of chemical reactions. The helper catalyst can simultaneously act as a director molecule, suppressing undesired reactions and thus increasing selectivity toward the desired reaction. These catalysts can be useful for a variety of chemical reactions including, in particular, the electrochemical conversion of CO.sub.2 or formic acid. The catalysts can also suppress H.sub.2 evolution, permitting electrochemical cell operation at potentials below RHE. Chemical processes and devices using the catalysts are also disclosed, including processes to produce CO, OH.sup.-, HCO.sup.-, H.sub.2CO, (HCO.sub.2).sup.-, H.sub.2CO.sub.2, CH.sub.3OH, CH.sub.4, C.sub.2H.sub.4, CH.sub.3CH.sub.2OH, CH.sub.3COO.sup.-, CH.sub.3COOH, C.sub.2H.sub.6, O.sub.2, H.sub.2, (COOH).sub.2, or (COO.sup.-).sub.2, and a specific device, namely, a CO.sub.2 sensor.

  12. Fundamental studies of the mechanism of catalytic reactions with catalysts effective in the gasification of carbon solids and the oxidative coupling of methane. Quarterly report, October 1, 1994--December 31, 1994

    Energy Technology Data Exchange (ETDEWEB)

    Iglesia, E.; Perry, D.L.; Heinemann, H.

    1994-12-01

    This report describes research on the oxidative coupling of methane and catalysts involved in coal gasification. Topics include methane pyrolysis and catalysts, and magnetic properties of the coal gasification catalyst Ca-Ni-K-O system.

  13. Dye-sensitized MIL-101 metal organic frameworks loaded with Ni/NiOx nanoparticles for efficient visible-light-driven hydrogen generation

    Directory of Open Access Journals (Sweden)

    Xin-Ling Liu

    2015-10-01

    Full Text Available The Ni/NiOx particles were in situ photodeposited on MIL-101 metal organic frameworks as catalysts for boosting H2 generation from Erythrosin B dye sensitization under visible-light irradiation. The highest H2 production rate of 125 μmol h−1 was achieved from the system containing 5 wt. % Ni-loaded MIL-101 (20 mg and 30 mg Erythrosin B dye. Moreover, the Ni/NiOx catalysts show excellent stability for long-term photocatalytic reaction. The enhancement on H2 generation is attributed to the efficient charge transfer from photoexcited dye to the Ni catalyst via MIL-101. Our results demonstrate that the economical Ni/NiOx particles are durable and active catalysts for photocatalytic H2 generation.

  14. Dye-sensitized MIL-101 metal organic frameworks loaded with Ni/NiO{sub x} nanoparticles for efficient visible-light-driven hydrogen generation

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Xin-Ling; Wang, Rong; Yuan, Yu-Peng, E-mail: yupengyuan@ahu.edu.cn, E-mail: cxue@ntu.edu.sg [School of Chemistry and Chemical Engineering, and Innovation Lab for Clean Energy and Green Catalysis, Anhui University, Hefei 230036 (China); Zhang, Ming-Yi [Key Laboratory for Photonic and Electronic Bandgap Materials, Ministry of Education, School of Physics and Electronic Engineering, Harbin Normal University, Harbin 150025 (China); Xue, Can, E-mail: yupengyuan@ahu.edu.cn, E-mail: cxue@ntu.edu.sg [Solar Fuels Lab, School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798 (Singapore)

    2015-10-01

    The Ni/NiO{sub x} particles were in situ photodeposited on MIL-101 metal organic frameworks as catalysts for boosting H{sub 2} generation from Erythrosin B dye sensitization under visible-light irradiation. The highest H{sub 2} production rate of 125 μmol h{sup −1} was achieved from the system containing 5 wt. % Ni-loaded MIL-101 (20 mg) and 30 mg Erythrosin B dye. Moreover, the Ni/NiO{sub x} catalysts show excellent stability for long-term photocatalytic reaction. The enhancement on H{sub 2} generation is attributed to the efficient charge transfer from photoexcited dye to the Ni catalyst via MIL-101. Our results demonstrate that the economical Ni/NiO{sub x} particles are durable and active catalysts for photocatalytic H{sub 2} generation.

  15. Novel anode catalyst for direct methanol fuel cells.

    Science.gov (United States)

    Basri, S; Kamarudin, S K; Daud, W R W; Yaakob, Z; Kadhum, A A H

    2014-01-01

    PtRu catalyst is a promising anodic catalyst for direct methanol fuel cells (DMFCs) but the slow reaction kinetics reduce the performance of DMFCs. Therefore, this study attempts to improve the performance of PtRu catalysts by adding nickel (Ni) and iron (Fe). Multiwalled carbon nanotubes (MWCNTs) are used to increase the active area of the catalyst and to improve the catalyst performance. Electrochemical analysis techniques, such as energy dispersive X-ray spectrometry (EDX), X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), and X-ray photoelectron spectroscopy (XPS), are used to characterize the kinetic parameters of the hybrid catalyst. Cyclic voltammetry (CV) is used to investigate the effects of adding Fe and Ni to the catalyst on the reaction kinetics. Additionally, chronoamperometry (CA) tests were conducted to study the long-term performance of the catalyst for catalyzing the methanol oxidation reaction (MOR). The binding energies of the reactants and products are compared to determine the kinetics and potential surface energy for methanol oxidation. The FESEM analysis results indicate that well-dispersed nanoscale (2-5 nm) PtRu particles are formed on the MWCNTs. Finally, PtRuFeNi/MWCNT improves the reaction kinetics of anode catalysts for DMFCs and obtains a mass current of 31 A g(-1) catalyst.

  16. Novel Anode Catalyst for Direct Methanol Fuel Cells

    Directory of Open Access Journals (Sweden)

    S. Basri

    2014-01-01

    Full Text Available PtRu catalyst is a promising anodic catalyst for direct methanol fuel cells (DMFCs but the slow reaction kinetics reduce the performance of DMFCs. Therefore, this study attempts to improve the performance of PtRu catalysts by adding nickel (Ni and iron (Fe. Multiwalled carbon nanotubes (MWCNTs are used to increase the active area of the catalyst and to improve the catalyst performance. Electrochemical analysis techniques, such as energy dispersive X-ray spectrometry (EDX, X-ray diffraction (XRD, field emission scanning electron microscopy (FESEM, and X-ray photoelectron spectroscopy (XPS, are used to characterize the kinetic parameters of the hybrid catalyst. Cyclic voltammetry (CV is used to investigate the effects of adding Fe and Ni to the catalyst on the reaction kinetics. Additionally, chronoamperometry (CA tests were conducted to study the long-term performance of the catalyst for catalyzing the methanol oxidation reaction (MOR. The binding energies of the reactants and products are compared to determine the kinetics and potential surface energy for methanol oxidation. The FESEM analysis results indicate that well-dispersed nanoscale (2–5 nm PtRu particles are formed on the MWCNTs. Finally, PtRuFeNi/MWCNT improves the reaction kinetics of anode catalysts for DMFCs and obtains a mass current of 31 A g−1 catalyst.

  17. Dates in the development of catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Simon

    1943-05-20

    A chronological listing is presented of the dates on which various I. G. Farbenindustrie catalysts were first used. In most cases the entries gave compositions and some hints at the methods of preparation of the catalysts as well as the code numbers for the catalysts. The listing started in December, 1924, and extended throught August, 1941. Some of the more important catalysts were the following: 5058, tungsten disulfide (WS/sub 2/), produced from the thio salt by dry decomposition (1930); 6434, a diluted mixture of hydrogen fluoride-treated ''Terrana'' and 10% WS/sub 2/ (1935); 6719, a prehydrogenation catalyst of 75 parts ferrous sulfide (FeS), 22 parts WS/sub 2/, and 3 parts nickel monosulfide (NiS) (1937); 7019, an aromatization catalyst of 100 parts primry coal, 15 parts chromic oxide (Cr/sub 2/O/sub 3/), and 5 parts vanadium sesquioxide (V/sub 2/O/sub 3/) (1938); 7360, a DHD catalyst of activated alumina (Al/sub 2/O/sub 3/) and 55 g/l molybdenum trioxide (MoO/sub 3/) (1939); 7846, a prehydrogenated catalyst, a sulfonated mixture of activated alumina, 100 g/l MoO/sub 3/, and 30 g/l nickel sesquioxide (Ni/sub 2/O/sub 3/) (1940); and 8376 W, a prehydrogenation catalyst, a sulfonated mixture of activated alumina, 250 g/l tungsten trioxide (WO/sub 3/), and 50 g/l Ni/sub 2/O/sub 3/ (1941). Other caalysts given included numbers 1724, 2365, 2473, 2500, 3510, 3884, 5053, 5676, 6525, and 6561. Compounds used other than those mentioned above included molybdenum disulfide (MoS/sub 2/), zinc sulfide (ZnS), zinc oxide (ZnO), and magnesium oxide (MgO).

  18. Highly dispersed metal catalyst

    Science.gov (United States)

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

    2016-11-08

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

  19. Facile synthesis of monodisperse thermally immiscible Ag–Ni alloy ...

    Indian Academy of Sciences (India)

    Administrator

    to their synergistic effects. Using Ag–Ni ANPs, at the same time, is more economical than pure silver ANPs. According to the literature, metal-catalyst decoration can .... 1451. Figure 7. Schematic representation of the Ag–Ni ANP forma- tion. M stands for a metal element. Schematic representation of the Ag–Ni ANP formation.

  20. Effect of Ni Core Structure on the Electrocatalytic Activity of Pt-Ni/C in Methanol Oxidation

    Science.gov (United States)

    Kang, Jian; Wang, Rongfang; Wang, Hui; Liao, Shijun; Key, Julian; Linkov, Vladimir; Ji, Shan

    2013-01-01

    Methanol oxidation catalysts comprising an outer Pt-shell with an inner Ni-core supported on carbon, (Pt-Ni/C), were prepared with either crystalline or amorphous Ni core structures. Structural comparisons of the two forms of catalyst were made using transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), and methanol oxidation activity compared using CV and chronoamperometry (CA). While both the amorphous Ni core and crystalline Ni core structures were covered by similar Pt shell thickness and structure, the Pt-Ni(amorphous)/C catalyst had higher methanol oxidation activity. The amorphous Ni core thus offers improved Pt usage efficiency in direct methanol fuel cells. PMID:28811402

  1. Effect of Ni Core Structure on the Electrocatalytic Activity of Pt-Ni/C in Methanol Oxidation

    Directory of Open Access Journals (Sweden)

    Vladimir Linkov

    2013-07-01

    Full Text Available Methanol oxidation catalysts comprising an outer Pt-shell with an inner Ni-core supported on carbon, (Pt-Ni/C, were prepared with either crystalline or amorphous Ni core structures. Structural comparisons of the two forms of catalyst were made using transmission electron microscopy (TEM, X-ray diffraction (XRD and X-ray photoelectron spectroscopy (XPS, and methanol oxidation activity compared using CV and chronoamperometry (CA. While both the amorphous Ni core and crystalline Ni core structures were covered by similar Pt shell thickness and structure, the Pt-Ni(amorphous/C catalyst had higher methanol oxidation activity. The amorphous Ni core thus offers improved Pt usage efficiency in direct methanol fuel cells.

  2. Catalyst Architecture

    DEFF Research Database (Denmark)

    Kiib, Hans; Marling, Gitte; Hansen, Peter Mandal

    2014-01-01

    How can architecture promote the enriching experiences of the tolerant, the democratic, and the learning city - a city worth living in, worth supporting and worth investing in? Catalyst Architecture comprises architectural projects, which, by virtue of their location, context and their combination...... of programs, have a role in mediating positive social and/or cultural development. In this sense, we talk about architecture as a catalyst for: sustainable adaptation of the city’s infrastructure appropriate renovation of dilapidated urban districts strengthening of social cohesiveness in the city development...

  3. A Review on Bimetallic Nickel-Based Catalysts for CO2 Reforming of Methane.

    Science.gov (United States)

    Bian, Zhoufeng; Das, Sonali; Wai, Ming Hui; Hongmanorom, Plaifa; Kawi, Sibudjing

    2017-11-17

    In recent years, CO2 reforming of methane (dry reforming of methane, DRM) has become an attractive research area because it converts two major greenhouse gasses into syngas (CO and H2 ), which can be directly used as fuel or feedstock for the chemical industry. Ni-based catalysts have been extensively used for DRM because of its low cost and good activity. A major concern with Ni-based catalysts in DRM is severe carbon deposition leading to catalyst deactivation, and a lot of effort has been put into the design and synthesis of stable Ni catalysts with high carbon resistance. One effective and practical strategy is to introduce a second metal to obtain bimetallic Ni-based catalysts. The synergistic effect between Ni and the second metal has been shown to increase the carbon resistance of the catalyst significantly. In this review, a detailed discussion on the development of bimetallic Ni-based catalysts for DRM including nickel alloyed with noble metals (Pt, Ru, Ir etc.) and transition metals (Co, Fe, Cu) is presented. Special emphasis has been provided on the underlying principles that lead to synergistic effects and enhance catalyst performance. Finally, an outlook is presented for the future development of Ni-based bimetallic catalysts. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  4. Hydrogen from ethylene glycol by supercritical water reforming supported noble and base metal catalysts

    NARCIS (Netherlands)

    de Vlieger, Dennis; Chakinala, A.G.; Lefferts, Leonardus; Kersten, Sascha R.A.; Seshan, Kulathuiyer; Brilman, Derk Willem Frederik

    2012-01-01

    Catalytic reforming of ethylene glycol (5 and 15 wt%) in supercritical water (450 °C and 250 bar) in the presence of alumina supported mono- and bi-metallic catalysts based on Ir, Pt and Ni was studied. Pt catalyst showed the highest hydrogen yields compared to Ir and Ni. Varying the Pt loading

  5. Alloy composition dependence of formation of porous Ni prepared by rapid solidification and chemical dealloying

    Energy Technology Data Exchange (ETDEWEB)

    Qi Zhen [Key Laboratory of Liquid Structure and Heredity of Materials, Shandong University, Jingshi Road 73, Jinan 250061 (China); Zhang Zhonghua [Key Laboratory of Liquid Structure and Heredity of Materials, Shandong University, Jingshi Road 73, Jinan 250061 (China)], E-mail: zh_zhang@sdu.edu.cn; Jia Haoling [Key Laboratory of Liquid Structure and Heredity of Materials, Shandong University, Jingshi Road 73, Jinan 250061 (China); Qu Yingjie [Shandong Labor Occupational Technology College, Jingshi Road 388, Jinan 250022 (China); Liu Guodong; Bian Xiufang [Key Laboratory of Liquid Structure and Heredity of Materials, Shandong University, Jingshi Road 73, Jinan 250061 (China)

    2009-03-20

    In this paper, the effect of alloy composition on the formation of porous Ni catalysts prepared by chemical dealloying of rapidly solidified Al-Ni alloys has been investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM) with energy dispersive X-ray (EDX) analysis and N{sub 2} adsorption experiments. The experimental results show that rapid solidification and alloy composition have a significant effect on the phase constituent and microstructure of Al-Ni alloys. The melt spun Al-20 at.% Ni alloy consists of {alpha}-Al, NiAl{sub 3} and Ni{sub 2}Al{sub 3}, while the melt spun Al-25 and 31.5 at.% Ni alloys comprise NiAl{sub 3} and Ni{sub 2}Al{sub 3}. Moreover, the formation and microstructure of the porous Ni catalysts are dependent upon the composition of the melt spun Al-Ni alloys. The morphology and size of Ni particles in the Ni catalysts inherit from those of grains in the melt spun Al-Ni alloys. Rapid solidification can extend the alloy composition of Al-Ni alloys suitable for preparation of the Ni catalysts, and obviously accelerate the dealloying process of the Al-Ni alloys.

  6. Preparation of Supported Metal Catalysts by Atomic and Molecular Layer Deposition for Improved Catalytic Performance

    Science.gov (United States)

    Gould, Troy D.

    Creating catalysts with enhanced selectivity and activity requires precise control over particle shape, composition, and size. Here we report the use of atomic layer deposition (ALD) to synthesize supported Ni, Pt, and Ni-Pt catalysts in the size regime (nanoparticles by depositing Ni on Al2O3 with two half-reactions of Ni(Cp)2 and H2. By changing the number of ALD cycles, Ni weight loadings were varied from 4.7 wt% to 16.7 wt% and the average particle sizes ranged from 2.5 to 3.3 nm, which increased the selectivity for C 3H6 hydrogenolysis by an order of magnitude over a much larger Ni/Al2O3 catalyst. Pt particles were deposited by varying the number of ALD cycles and the reaction chemistry (H2 or O 2) to control the particle size from approximately 1 to 2 nm, which allowed lower-coordinated surface atoms to populate the particle surface. These Pt ALD catalysts demonstrated some of the highest oxidative dehydrogenation of propane selectivities (37%) of a Pt catalyst synthesized by a scalable technique. Dry reforming of methane (DRM) is a reaction of interest due to the recent increased recovery of natural gas, but this reaction is hindered from industrial implementation because the Ni catalysts are plagued by deactivation from sintering and coking. This work utilized Ni ALD and NiPt ALD catalysts for the DRM reaction. These catalysts did not form destructive carbon whiskers and had enhanced reaction rates due to increased bimetallic interaction. To further limit sintering, the Ni and NiPt ALD catalysts were coated with a porous alumina matrix by molecular layer deposition (MLD). The catalysts were evaluated for DRM at 973 K, and the MLD-coated Ni catalysts outperformed the uncoated Ni catalysts in either activity (with 5 MLD cycles) or stability (with 10 MLD cycles). In summary, this thesis developed a new Ni nanoparticle ALD chemistry, explored possibilities for changing Pt ALD particle size, brought the two techniques together to create enhanced bimetallic

  7. A CATALYST, A PROCESS FOR SELECTIVE HYDROGENATION OF ACETYLENE TO ETHYLENE AND A METHOD FOR THE MANUFACTURE OF THE CATALYST

    DEFF Research Database (Denmark)

    2009-01-01

    A catalyst comprising a mixture of metal A selected from the group of Fe, Co and Ni and metal B selected from the group of Zn and Ga, and a support material, wherein the two metals are present in an intermetallic composition; A method for the manufacture of the catalyst; and the use of above...

  8. Coal catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Kroenig, W.

    1944-02-11

    Some considerations in the selection of a catalyst for the liquid phase of coal hydrogenation are discussed. Some of the previous history of such selections is mentioned. At one stage of the development, the principal catalyst had been iron sulfate (FeSO/sub 4/.7H/sub 2/O). Later, for reasons of cost and availability of large supplies, selections had turned to mixtures of iron sulfate and one or another of some iron oxide- and aluminum oxide-containing byproducts of aluminum manufacture, namely Bayermasse, Luxamsse, or Lautamasse. Much of the discussion centered on optimal proportions for such mixtures, particularly as related to pH values of resulting coal pastes. Upper Silesian coal was more alkaline than Ruhr coal, and Bayermasse, etc., were quite alkaline. Thus, since the iron sulfate served as a partial neutralizer for the coal as well as a catalyst, it seemed necessary to increase the proportions of iron sulfate in the catalyst mixture when processing coal of greater alkalinity. A further reason for a greater proportion of iron sulfate seemed to be that most of the catalytic activity of the iron came from the ferrous iron of iron sulfate rather than from the ferric iron of the other materials. Ferrous-ferric ratios also seemed to indicate that Luxmasse or Lautamasse might be better catalyst components than Bayermasse but their water content sometimes caused handling problems, so Bayermasse had been more widely used. Formation of deposits in the preheater was more likely due to the Bayermasse than to the iron sulfate; sodium sulfide could help to prevent them.

  9. Enhanced MEA Performance for PEMFCs under Low Relative Humidity and Low Oxygen Content Conditions via Catalyst Functionalization

    Energy Technology Data Exchange (ETDEWEB)

    Xin, Le; Yang, Fan; Xie, Jian; Yang, Zhiwei; Kariuki, Nancy N.; Myers, Deborah J.; Peng, Jui-Kun; Wang, Xiaohua; Ahluwalia, Rajesh K.; Yu, Kang; Ferreira, Paulo J.; Bonastre, Alex Martinez; Fongalland, Dash; Sharman, Jonathan

    2017-01-01

    This work demonstrates that functionalizing annealed-Pt/Ketjen black EC300j (a-Pt/KB) and dealloyed-PtNi/Ketjen black EC300j (d-PtNi/KB) catalysts using p-phenyl sulfonic acid can effectively enhance performance in the membrane electrode assemblies (MEAs) of proton exchange membrane fuel cells (PEMFCs). The functionalization increased the size of both Pt and PtNi catalyst particles and resulted in the further leaching of Ni from the PtNi catalyst while promoting the formation of nanoporous PtNi nanoparticles. The size of the SO3H-Pt/KB and SO3H-PtNi/KB carbon-based aggregates decreased dramatically, leading to the formation of catalyst layers with narrower pore size distributions.MEA tests highlighted the benefits of the surface functionalization, in which the cells with SO3H-Pt/KB and SO3H-PtNi/KB cathode catalysts showed superior high current density performance under reduced RH conditions, in comparison with cells containing annealed Pt/KB (a-Pt/KB) and de-alloyed PtNi/KB (d-PtNi/KB) catalysts. The performance improvement was particularly evident when using reactant gases with low relative humidity, indicating that the hydrophilic functional groups on the carbon improved the water retention in the cathode catalyst layer. These results show a new avenue for enhancing catalyst performance for the next generation of catalytic materials for PEMFCs.

  10. Microwave assisted synthesis and characterization of Ni/NiO nanoparticles as electrocatalyst for methanol oxidation in alkaline solution

    Science.gov (United States)

    Arunachalam, Prabhakarn; Ghanem, Mohamed A.; Al-Mayouf, Abdullah M.; Al-shalwi, Matar; Hamed Abd-Elkader, Omar

    2017-02-01

    Nickel/Nickel oxide (Ni/NiO) nanoparticles catalyst is prepared by microwave-assisted liquid-phase deposition using ethylene glycol (EG) and water mixture under atmospheric conditions. The physicochemical characterizations of the catalyst carried out by surface area analyzer, x-ray diffraction (XRD), x-ray photoelectron spectroscopy (XPS), electron microscopes measurements suggest the formation of crystalline nanoparticles structure of NiO. The surface area of Ni/NiO prepared using EG/water mixture reaches 70 m2 g-1 which is 2-fold enhsancement in surface area in comparison with NiO prepared in pure EG and an order of magnitude higher than that of bulk nickel prepared in pure water. The methanol electro-oxidation activity of the Ni/NiO nanoparticles obtained in EG/water mixture displayed more than 4-fold increase in oxidation current at 1.7 V versus RHE in comparison with NiO nanoparticles obtained in EG and 20-fold increase compared to bulk nickel catalyst concord with the enhancement of electro-active surface area. The results show the Ni/NiO nanoparticles produced by microwave assisted synthesis has superior activity for methanol oxidation in alkaline solution over the other nickel based catalysts and has potential for mass production.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-05-25

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

  12. Low temperature catalyst system for methanol production

    Science.gov (United States)

    Sapienza, R.S.; Slegeir, W.A.; O'Hare, T.E.

    1984-04-20

    This patent discloses a catalyst and process useful at low temperatures (150/sup 0/C) and preferably in the range 80 to 120/sup 0/C used in the production of methanol from carbon monoxide and hydrogen. The catalyst components are used in slurry form and comprise (1) a complex reducing agent derived from the component structure NaH-ROH-M(OAc)/sub 2/ where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1 to 6 carbon atoms and (2) a metal carbonyl of a group VI (Mo, Cr, W) metal. For the first component, Nic is preferred (where M = Ni and R = tertiary amyl). For the second component, Mo(CO)/sub 6/ is preferred. The mixture is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

  13. Low temperature catalysts for methanol production

    Science.gov (United States)

    Sapienza, Richard S.; Slegeir, William A.; O'Hare, Thomas E.; Mahajan, Devinder

    1986-01-01

    A catalyst and process useful at low temperatures (below about 160.degree. C.) and preferably in the range 80.degree.-120.degree. C. used in the production of methanol from carbon monoxide and hydrogen is disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH--RONa--M(OAc).sub.2 where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1-6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is Nic (where M=Ni and R=tertiary amyl). Mo(CO).sub.6 is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

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

    Energy Technology Data Exchange (ETDEWEB)

    Suljo Linic

    2008-12-31

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

  15. Modification of the performance of WO3-ZrO2 catalysts by metal addition in hydrocarbon reactions

    Directory of Open Access Journals (Sweden)

    Gerardo Carlos Torres

    2012-01-01

    Full Text Available A study of the different hydrocarbon reactions over Ni doped WO3-ZrO2 catalysts was performed. Ni was found as NiO at low Ni concentration while at high Ni concentrations a small fraction was present as a metal. For both cases, Ni strongly modified total acidity and concentration of strong acid sites. In the cyclohexane dehydrogenation reaction, Ni addition promotes both benzene and methyl cyclopentane production. The hydroconversion activity (n-butane and n-octane increases with the augment of total acidity produced by Ni. The selectivity to reaction products is modified according to the acid strength distribution changes produced by Ni addition.

  16. Synthesis and Characterization of Carbon Nanotubes Catalyzed by TiO2 Supported Ni, Co and Ni-Co Nanoparticles via CCVD

    Directory of Open Access Journals (Sweden)

    A. A. Hosseini

    2013-09-01

    Full Text Available Monometallic and bimetallic Ni and Co catalytic nanoparticles supported on Titanium dioxide (rutile phase substrate were prepared by wet impregnation method. These nanoparicles were used as catalysts for synthesis of multiwalled carbon nanotubes (MWCNTs from acetylene decomposition at 700°C by the catalytic chemical vapor deposition (CCVD technique. The nanomaterials (catalyst and CNTs were characterized by X-ray diffraction (XRD, Scanning electron microscopy (SEM and Raman spectroscopy. In this paper, the usage of TiO2 powder as catalyst support was examined and the effect of applied catalyst type on characteristics of grown CNTs was investigated. The results showed that the rutile phase of TiO2 powder can be applied as a suitable catalyst support in CNT growth process. Furthermore, it was observed that the CNTs synthesized on Ni-Co bimetallic catalyst possess smaller average diameters, better quality and less amorphous carbon compared to Ni and Co monometallic catalyst types.

  17. In situ Transmission Electron Microscopy of catalyst sintering

    DEFF Research Database (Denmark)

    DeLaRiva, Andrew T.; Hansen, Thomas Willum; Challa, Sivakumar R.

    2013-01-01

    along with our recent in situ TEM studies on the sintering of Ni/MgAl2O4 catalysts. These results suggest that the rapid loss of catalyst activity in the earliest stages of catalyst sintering could result from Ostwald ripening rather than through particle migration and coalescence. The smallest...... of Ostwald ripening as well as atomistic Monte Carlo simulations are both in good agreement with these experimental observations, predicting a steep loss in catalyst activity at short times on stream. The in situ studies show the importance of direct observations to deduce mechanisms and show the important...

  18. Hydrogen production from bio-fuels using precious metal catalysts

    Science.gov (United States)

    Pasel, Joachim; Wohlrab, Sebastian; Rotov, Mikhail; Löhken, Katrin; Peters, Ralf; Stolten, Detlef

    2017-11-01

    Fuel cell systems with integrated autothermal reforming unit require active and robust catalysts for H2 production. Thus, an experimental screening of catalysts for autothermal reforming of commercial biodiesel fuel was performed. Catalysts consisted of a monolithic cordierite substrate, an oxide support (γ-Al2O3) and Pt, Ru, Ni, PtRh and PtRu as active phase. Experiments were run by widely varying the O2/C and H2O/C molar ratios at different gas hourly space velocities. Fresh and aged catalysts were characterized by temperature programmed methods and thermogravimetry to find correlations with catalytic activity and stability.

  19. Hydrogen production from bio-fuels using precious metal catalysts

    Directory of Open Access Journals (Sweden)

    Pasel Joachim

    2017-01-01

    Full Text Available Fuel cell systems with integrated autothermal reforming unit require active and robust catalysts for H2 production. Thus, an experimental screening of catalysts for autothermal reforming of commercial biodiesel fuel was performed. Catalysts consisted of a monolithic cordierite substrate, an oxide support (γ-Al2O3 and Pt, Ru, Ni, PtRh and PtRu as active phase. Experiments were run by widely varying the O2/C and H2O/C molar ratios at different gas hourly space velocities. Fresh and aged catalysts were characterized by temperature programmed methods and thermogravimetry to find correlations with catalytic activity and stability.

  20. Single chamber microbial fuel cell with Ni-Co cathode

    Science.gov (United States)

    Włodarczyk, Barbara; Włodarczyk, Paweł P.; Kalinichenko, Antonina

    2017-10-01

    The possibility of wastewater treatment and the parallel energy production using the Ni-Co alloy as cathode catalyst for single chamber microbial fuel cells is presented in this research. The research included a preparation of catalyst and comparison of COD, NH4+ and NO3- reduction in the reactor without aeration, with aeration and with using a single chamber microbial fuel cell with Ni-Co cathode. The reduction time for COD with the use of microbial fuel cell with the Ni-Co catalyst is similar to the reduction time with aeration. The current density (2.4 A·m-2) and amount of energy (0.48 Wh) obtained in MFC is low, but the obtained amount of energy allows elimination of the energy needed for reactor aeration. It has been shown that the Ni-Co can be used as cathode catalyst in single chamber microbial fuel cells.

  1. Catalysts, Protection Layers, and Semiconductors

    DEFF Research Database (Denmark)

    Chorkendorff, Ib

    2015-01-01

    acid or alkaline conditions. Since most relevant semiconductors are very prone to corrosion the advantage of using buried junctions and using protection layers offering shall be discussed [2-4]. Next we shall discuss the availability of various catalysts for being coupled to these protections layers...... and how their stability may be evaluated [5, 6]. Examples of half-cell reaction using protection layers for both cathode and anode will be discussed though some of recent examples under both alkaline and acidic conditions. Si is a very good low band gap semiconductor and by using TiO2 as a protection...... layer we can stabilize it for both H2 and O2 evolution [7, 8, 9, 10]. Notably NiOx promoted by iron is a material that is transparent, providing protection, and is a good catalyst for O2 evolution. We have also recently started searching for large band gap semicondutors like III-V based or pervoskite...

  2. Ni nanoparticles prepared by simple chemical method for the synthesis of Ni/NiO-multi-layered graphene by chemical vapor deposition

    Science.gov (United States)

    Ali, Mokhtar; Remalli, Nagarjuna; Gedela, Venkataramana; Padya, Balaji; Jain, Pawan Kumar; Al-Fatesh, Ahmed; Rana, Usman Ali; Srikanth, Vadali V. S. S.

    2017-02-01

    A new chemical method was used to obtain a high yield of nickel nanoparticles (Ni-NPs). The effect of solvent (distilled water, ethylene glycol, and ethanol) and surfactant (oleic acid and polyvinyl pyrrolidinone) on the morphology and crystallinity of the synthesized Ni-NPs has been investigated. The experimental results revealed that among the solvents mentioned above, ethanol gives the best results in terms of complete reduction, controlled morphology and size distribution of Ni-NPs. The surfactants played an important role in impeding the agglomeration and surface oxidation of Ni-NPs. The surfactants also affected the morphology of the Ni-NPs. The synthesized Ni-NPs are found to be quite stable in air. The best of the synthesized Ni-NPs were effectively used as catalysts for the synthesis of Ni/NiO-multi-layered graphene using catalytic chemical vapor deposition technique.

  3. Attrition resistant fluidizable reforming catalyst

    Science.gov (United States)

    Parent, Yves O [Golden, CO; Magrini, Kim [Golden, CO; Landin, Steven M [Conifer, CO; Ritland, Marcus A [Palm Beach Shores, FL

    2011-03-29

    A method of preparing a steam reforming catalyst characterized by improved resistance to attrition loss when used for cracking, reforming, water gas shift and gasification reactions on feedstock in a fluidized bed reactor, comprising: fabricating the ceramic support particle, coating a ceramic support by adding an aqueous solution of a precursor salt of a metal selected from the group consisting of Ni, Pt, Pd, Ru, Rh, Cr, Co, Mn, Mg, K, La and Fe and mixtures thereof to the ceramic support and calcining the coated ceramic in air to convert the metal salts to metal oxides.

  4. Synthesis, characterization and catalytic activity of nanosized Ni complexed aminoclay

    Science.gov (United States)

    Ranchani, A. Amala Jeya; Parthasarathy, V.; Devi, A. Anitha; Meenarathi, B.; Anbarasan, R.

    2017-11-01

    A novel Ni complexed aminoclay (AC) catalyst was prepared by complexation method followed by reduction reaction. Various analytical techniques such as FTIR spectroscopy, UV-visible spectroscopy, DSC, TGA, SEM, HRTEM, EDX, XPS and WCA measurement are used to characterize the synthesized material. The AC-Ni catalyst system exhibited improved thermal stability and fiber-like morphology. The XPS results declared the formation of Ni nanoparticles. Thus, synthesized catalyst was tested towards the Schiff base formation reaction between various bio-medical polymers and aniline under air atmosphere at 85 °C for 24 h. The catalytic activity of the catalyst was studied by varying the % weight loading of the AC-Ni system towards the Schiff base formation. The Schiff base formation was quantitatively calculated by the 1H-NMR spectroscopy. While increasing the % weight loading of the AC-Ni catalyst, the % yield of Schiff base was also increased. The k app and Ti values were determined for the reduction of indole and α-terpineol in the presence of AC-Ni catalyst system. The experimental results were compared with the literature report.

  5. Effects of chelating agents as additives on preparation of Co-Mo hydrodesulfurization catalysts. Effect of NTA (Nitrilotriacetic acid) addition on hydrodesulfurization activity and surface composition; Co-Mo kei datsuryu shokubai choseiji ni okeru kiretozai no tenka koka. Datsuryu kassei to hyomen sosei ni taisuru NTA (nitoriro sansakusan) no tenka koka

    Energy Technology Data Exchange (ETDEWEB)

    Shimizu, T.; Kasahara, S.; Kiyohara, T.; Kawahara, K.; Yamada, M. [Tohoku University, Sendai (Japan). Faculty of Engineering

    1995-11-01

    Co-Mo/Al2O3 catalysts prepared by an impregnation method using NTA (nitrilotriacetic acid) as a chelating agent, were used to test the hydrodesulfurization (HDS) activity of benzothiophene and to observe the effect of XPS (X-ray photoelectron spectroscopy). The NTA-added catalysts showed ca. 20% higher HDS activity than that of conventional catalysts. The result of the activity test as a function of Co/Mo ratio suggested that the same highly active sites were formed when Co/Mo ratio (atom/atom) was less than ca. 0.3, and above 0.3 less active Co species was formed. It was also suggested that NTA contributed to the formation and to increasing the number of highly alive sites. When the NTA-added catalysts were calcined before sulfidation, the increment of HDS acidity was reduced by half. XPS measurements for catalyst precursors (before sulfidation) revealed that, when they were not calcined, the Co concentration at the surface of the catalysts prepared by the NTA method was higher than that of the conventionally prepared catalysts. Accordingly, it was suggested that NTA has a role of increasing Co surface density; thus, increasing the catalytic activity. 18 refs., 7 figs., 1 tab.

  6. Seed-mediated synthesis of cross-linked Pt-NiO nanochains for methanol oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Gu, Zhulan; Bin, Duan; Feng, Yue; Zhang, Ke; Wang, Jin; Yan, Bo; Li, Shumin; Xiong, Zhiping; Wang, Caiqin; Shiraishi, Yukihide; Du, Yukou, E-mail: duyk@suda.edu.cn

    2017-07-31

    Highlights: • Cross-linked Pt-NiO nanochains using seed-mediated growth method are synthesized. • The as-prepared catalysts exhibit higher electrocatalytic activity than Pt/C for MOR. • The Pt-NiO(1:1 by molar) catalyst shows the best electrocatalytic property towards MOR. - Abstract: A simple method was reported for employing NiO nanoparticles act as seeds and then different amounts of Pt{sup 2+} were reduced on the NiO nanoparticles, forming a cross-linked Pt-NiO nanocatalysts. These as-prepared catalysts were characterized using different physical-chemical techniques, including X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The results indicate that the morphology of the cross-linked Pt-NiO nanochain was successfully produced regardless of the molar ratio of Pt{sup 2+} to NiO precursors. The electrochemical characteristics of Pt-NiO nanochain catalysts were evaluated for the oxidation of methanol as a model reaction, which verify that the Pt-NiO catalysts show enhanced activity and high stability in comparison with the commercial Pt/C catalyst. The optimized ratio of Pt to NiO is 1:1, then tuned by simple adjusting the feed ratio of the precursors as well. The synthesized nanocatalysts will be found the great potential applications as electrocatalysts for fuel cells owe to their enhanced catalytic performance and long-term stability.

  7. HYDROGENATION OF TOLUENE ON Ni-Co-Mo SUPPORTED ...

    African Journals Online (AJOL)

    HOD

    The activity results showed that toluene conversion of almost 100% and selectivity to mainly methyl-cyclohexane was achieved. The catalysts activity test showed that the zeolite support textural properties particularly surface area, pore volume and pore diameter affect the performance of the catalysts. NiCoMo/HY-b.

  8. Magnetism for understanding catalyst analysis of purified carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-08-01

    The precise quantification of catalyst residues in purified carbon nanotubes is often a major issue in view of any fundamental and/or applicative studies. More importantly, since the best CNTs are successfully grown with magnetic catalysts, their quantification becomes strictly necessary to better understand intrinsic properties of CNT. For these reasons, we have deeply analyzed the catalyst content remained in nickel–yttrium arc-discharge single walled carbon nanotubes purified by both a chlorine-gas phase and a standard acid-based treatment. The study focuses on Ni analysis which has been investigated by transmission electron microscopy, X-ray diffraction, thermogravimetry analysis, and magnetic measurements. In the case of the acid-based treatment, all quantifications result in a decrease of the nanocrystallized Ni by a factor of two. In the case of the halogen gas treatment, analysis and quantification of Ni content is less straightforward: a huge difference appears between X-ray diffraction and thermogravimetry results. Thanks to magnetic measurements, this disagreement is explained by the presence of Ni{sup 2+} ions, belonging to NiCl{sub 2} formed during the Cl-based purification process. In particular, NiCl{sub 2} compound appears under different magnetic/crystalline phases: paramagnetic or diamagnetic, or well intercalated in between carbon sheets with an ordered magnetic phase at low temperature. - Highlights: • Cl-gas treatment of Ni catalyst of carbon nanotubes leads to NiCl{sub 2} residue. • Magnetic measurements show the transformation of Ni{sup 0} in Ni{sup 2+}through a purification process. • High temperature Cl treatment removes 75% of metallic impurities. • Cl-purification yields to an amount of metal of 1.5% in arc-discharge CNT samples.

  9. Releasing metal catalysts via phase transition: (NiO)0.05-(SrTi0.8Nb0.2O3)0.95 as a redox stable anode material for solid oxide fuel cells.

    Science.gov (United States)

    Xiao, Guoliang; Wang, Siwei; Lin, Ye; Zhang, Yanxiang; An, Ke; Chen, Fanglin

    2014-11-26

    Donor-doped perovskite-type SrTiO3 experiences stoichiometric changes at high temperatures in different Po2 involving the formation of Sr or Ti-rich impurities. NiO is incorporated into the stoichiometric strontium titanate, SrTi0.8Nb0.2O3-δ (STN), to form an A-site deficient perovskite material, (NiO)0.05-(SrTi0.8Nb0.2O3)0.95 (Ni-STN), for balancing the phase transition. Metallic Ni nanoparticles can be released upon reduction instead of forming undesired secondary phases. This material design introduces a simple catalytic modification method with good compositional control of the ceramic backbones, by which transport property and durability of solid oxide fuel cell anodes are largely determined. Using Ni-STN as anodes for solid oxide fuel cells, enhanced catalytic activity and remarkable stability in redox cycling have been achieved. Electrolyte-supported cells with the cell configuration of Ni-STN-SDC anode, La0.8Sr0.2Ga0.87Mg0.13O3 (LSGM) electrolyte, and La0.6Sr0.4Co0.2Fe0.8O3 (LSCF) cathode produce peak power densities of 612, 794, and 922 mW cm(-2) at 800, 850, and 900 °C, respectively, using H2 as the fuel and air as the oxidant. Minor degradation in fuel cell performance resulted from redox cycling can be recovered upon operating the fuel cells in H2. Such property makes Ni-STN a promising regenerative anode candidate for solid oxide fuel cells.

  10. Resin catalysts and method of preparation

    Science.gov (United States)

    Smith, L.A. Jr.

    1986-12-16

    Heat stabilized catalyst compositions are prepared from nuclear sulfonic acid, for example, macroporous crosslinked polyvinyl aromatic compounds containing sulfonic acid groups are neutralized with a metal of Al, Fe, Zn, Cu, Ni, ions or mixtures and alkali, alkaline earth metals or ammonium ions by contacting the resin containing the sulfonic acid with aqueous solutions of the metals salts and alkali, alkaline earth metal or ammonium salts. The catalysts have at least 50% of the sulfonic acid groups neutralized with metal ions and the balance of the sulfonic acid groups neutralized with alkali, alkaline earth ions or ammonium ions.

  11. The Influence of Deposition Methods of Support Layer on Cordierite Substrate on the Characteristics of a MnO2–NiO–Co3O4/Ce0.2Zr0.8O2/Cordierite Three Way Catalyst

    Directory of Open Access Journals (Sweden)

    Phuong Thi Mai Pham

    2014-09-01

    Full Text Available This paper compares different coating methods (in situ solid combustion, hybrid deposition, secondary growth on seed, suspension, double deposition of wet impregnation and suspension to deposit Ce0.2Zr0.8O2 mixed oxides on cordierite substrates, for use as a three way catalyst. Among them, the double deposition was proven to be the most efficient one. The coated sample shows a BET (Brunauer–Emmett–Teller surface area of 25 m2/g, combined with a dense and crack free surface. The catalyst with a layer of MnO2–NiO–Co3O4 mixed oxides on top of the Ce0.2Zr0.8O2/cordierite substrate prepared by this method exhibits good activity for the treatment of CO, NO and C3H6 in exhaust gases (CO conversion of 100% at 250 °C, C3H6 conversion of 100% at 400 °C and NO conversion of 40% at 400 °C.

  12. Chemical interactions in multimetal/zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Sachtler, W.M.H.

    1992-02-07

    For Pt/NaY catalysts our analysis of the mechanism of metal particle formation has enabled us to produce at will samples which contain either the majority of the Pt particles in supercages, without filling these cages completely, or the Pt particles bulge into neighboring cages. The catalytic selectivity is distinctly different for these preparations, in the former case molecules can enter a supercage which is partially filled by the Pt cluster, in the second case adsorption takes place through the cage window. Applying the same principles of catalyst preparation of bimetallic catalysts enables us to produce PtCu particles in supercages of NaY, which contain, initially a Pt core, surrounded by a Cu mantle. Earlier we have found that Ni ions migrate into hexagonal prisms during calcination of Ni/NaY; this process can be partially suppressed by first filling these prisms with Mn or Cr ions. In more recent work we found that addition of Pt strongly lowers the temperature of Ni reduction. Part of the Ni ions is reduced by hydrogen while still inside the smaller cages. This reduction process is, however, reversible; at elevated temperature and in an inert atmosphere protons re-oxidize the Ni atoms and dihydrogen gas is developed. In this way it seems possible to count the Ni atoms in small cages. The calcination stage in the preparation of zeolite supported metals has been studied in considerable detail for Pd/NaY. The Pd is introduced as a tetrammin complex; during calcination the ammine ligands are successively oxidized. Once three ammine ligands are destroyed, the Pd ions which carry only one ligand, surprisingly jump from the supercages to the sodalite cage.

  13. Effects of chelating agents as additives on preparation of Co-Mo hydrodesulfurization catalysts. Part 2. Effect of nitrilotriacetic acid addition on surface structure; Co-Mo kei datsuryushokubai choseiji ni okeru chelate zai no tenka koka. 2. Hyomen kozo ni oyobosu nitrilo san sakusan tenka no eikyo

    Energy Technology Data Exchange (ETDEWEB)

    Shimizu, T.; Kiyohara, T.; Hiroshima, K.; Yamada, M. [Tohoku University, Sendai (Japan). Faculty of Engineering

    1996-03-01

    For the purpose of uncovering the cause of increased hydrodesulfurization (HDS) activity of Co-Mo/Al2O3 by the addition of nitrilotriacetic acid (NTA), the effects of order in adding NTA and the amount thereof on benzothiophene (BT) HDS activity were investigated. Effects of pretreatment condition were also studied, and it appeared that NTA did nor affect the optimum pretreatment condition. From the view of the surface structure, XPS was measured for the catalyst precursors, Mo EXAFS, FT-IR of adsorbed nitric oxide (NO), and the amount of NO adsorbed were measured for the sulfided catalysts, respectively. The XP spectra showed some concentration of Co at the surface of the catalyst precursor prepared with NTA. From the result of Mo EXAFS, it was thought that, when NTA was added during preparation, the growth of MoS2-like crystallite or the extent of crystallization was promoted. The IR spectra of NO adsorbed on sulfided catalysts showed that the adsorbed NO was mainly located on Co site. It was hence suggested that the addition of NTA promoted the coverage of Mo site with Co, and that the Co might have contributed toward the high HDS activity. The amount of NO adsorbed was found smaller for NTA-added catalyst than for the one prepared without NTA. Since the BT HDS activity was higher for NTA-added catalyst, it was thought that the addition of NTA might have promoted the formation of highly active sites. 14 refs., 7 figs., 3 tabs.

  14. Catalytic dehydrogenation of isobutane in the presence of hydrogen over Cs-modified Ni2P supported on active carbon

    Science.gov (United States)

    Xu, Yanli; Sang, Huanxin; Wang, Kang; Wang, Xitao

    2014-10-01

    In this article, an environmentally friendly non-noble-metal class of Cs-Ni2P/active carbon (AC) catalyst was prepared and demonstrated to exhibit enhanced catalytic performance in isobutane dehydrogenation. The results of activity tests reveal that Ni/AC catalyst was highly active for isobutane cracking, which led to the formation of abundant methane and coke. After the introduction of phosphorus through impregnation with ammonium di-hydrogen phosphate and H2-temperature programmed reduction, undesired cracking reactions were effectively inhibited, and the selectivity to isobutene and stability of catalyst increased remarkably. The characterization results indicate that, after the addition of phosphorous, the improvement of dehydrogenation selectivity is ascribed to the partial positive charges carried on Ni surface in Ni2P particles, which decreases the strength of Nisbnd C bond between Ni and carbonium-ion intermediates and the possibility of excessive dehydrogenation. In addition, Cs-modified Ni2P/AC catalysts display much higher catalytic performance as compared to Ni2P/AC catalyst. Cs-Ni2P-6.5 catalyst has the highest catalytic performance, and the selectivity to isobutene higher than 93% can be obtained even after 4 h reaction. The enhancement in catalytic performance of the Cs-modified catalysts is mainly attributed to the function of Cs to improve the dispersion of Ni2P particles, transfer electron from Cs to Ni, and decrease acid site number and strength.

  15. Combining Ru, Ni and Ni(OH){sub 2} active sites for improving catalytic performance in benzene hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Zhu, Lihua, E-mail: lihuazhu@stu.xmu.edu.cn [School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, Jiang Xi (China); Department of Chemical and Biochemical Engineering, National Engineering Laboratory for Green Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 (China); Sun, Hanlei; Zheng, Jinbao [Department of Chemical and Biochemical Engineering, National Engineering Laboratory for Green Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 (China); Yu, Changlin, E-mail: yuchanglinjx@163.com [School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, Jiang Xi (China); Zhang, Nuowei [Department of Chemical and Biochemical Engineering, National Engineering Laboratory for Green Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 (China); Shu, Qing [School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, Jiang Xi (China); Chen, Bing H., E-mail: chenbh@xmu.edu.cn [Department of Chemical and Biochemical Engineering, National Engineering Laboratory for Green Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 (China)

    2017-05-01

    In this study, the Ru{sub 0.04}Ni{sub 0.96}/C(T) catalysts were successfully prepared by the simple methods of hydrazine-reduction and galvanic replacement, where 0.04/0.96 and T represented the Ru/Ni atomic ratio and reducing temperature of the catalyst in N{sub 2}+10%H{sub 2}, respectively. The nanostructures of the Ru{sub 0.04}Ni{sub 0.96} nanoparticles in the Ru{sub 0.04}Ni{sub 0.96}/C(T) catalysts were controlled by modulating their annealing temperature in N{sub 2}+10%H{sub 2} and characterized by an array of techniques, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy energy dispersive X-ray spectroscopy (STEM-EDS) mapping and high-sensitivity low-energy ion scattering (HS-LEIS). The Ru{sub 0.04}Ni{sub 0.96}/C(30) catalyst, which was composed of Ru clusters or single atoms supported on Ni/Ni(OH){sub 2} nanoparticles, exhibited much better catalytic performance for benzene hydrogenation than the Ru{sub 0.04}Ni{sub 0.96}/C(T) catalysts reduced at above 30 °C, such as Ru{sub 0.04}Ni{sub 0.96}/C(160) with the nanostructure of partial Ru{sub 0.04}Ni{sub 0.9} alloy and Ru{sub 0.04}Ni{sub 0.96}/C(280) with the nanostructure of complete Ru{sub 0.04}Ni{sub 0.9} alloy. The reason was that the synergistic effect of multiple active sites – Ru, Ni and Ni(OH){sub 2} sites was present in the Ru{sub 0.04}Ni{sub 0.96}/C(30) catalyst, where hydrogen was preferentially activated at Ru sites, benzene was probably activated at Ni(OH){sub 2} surface and Ni acted as a “bridge” for transferring activated H{sup ∗} species to activated benzene by hydrogen spillover effect, hydrogenating and forming product – cyclohexane. This study also provided a typical example to illustrate that the synergy effect of multiple active sites can largely improve the catalytic hydrogenation performance. - Highlights: • The Ru

  16. Nickel-based xerogel catalysts: Synthesis via fast sol-gel method and application in catalytic hydrogenation of p-nitrophenol to p-aminophenol

    Science.gov (United States)

    Feng, Jin; Wang, Qiang; Fan, Dongliang; Ma, Lirong; Jiang, Deli; Xie, Jimin; Zhu, Jianjun

    2016-09-01

    In order to investigate the roles of three-dimensional network structure and calcium on Ni catalysts, the Ni, Ni-Al2O3, Ni-Ca-Al2O3 xerogel catalysts were successfully synthesized via the fast sol-gel process and chemical reduction method. The crystal structure of three different catalysts was observed with X-ray powder diffraction (XRD). Transmission electron microscopy (TEM), scanning electron microscopy (SEM) and nitrogen adsorption-desorption were employed to investigate the role of network structure of xerogel catalysts and the size distribution of Ni nanoparticles. The catalyst composition was determined by inductively coupled plasma-optical emission spectrometry (ICP-OES) measurement and energy-dispersive X-ray spectroscopy (EDS). Temperature-programmed reduction (TPR) experiments were carried out to investigate the reducibility of nickel species and the interaction between nickel species and alumina. The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over the prepared nickel-based xerogel catalysts. The conversion of p-nitrophenol was monitored by UV spectrophotometry and high performance liquid chromatography (HPLC). The results show that the catalysts are highly selective for the conversion of p-nitrophenol to p-aminophenol and the order of catalytic activities of the catalysts is Ni < Ni-Al2O3 < Ni-Ca-Al2O3. The catalysts were recycled and were used to evaluate the reutilization.

  17. Hydrogen production by auto-thermal reforming of ethanol over nickel catalyst supported on metal oxide-stabilized zirconia

    Energy Technology Data Exchange (ETDEWEB)

    Youn, Min Hye; Seo, Jeong Gil; Song, In Kyu [School of Chemical and Biological Engineering, Institute of Chemical Processes, Seoul National University, Shinlim-dong, Kwanak-ku, Seoul 151-744 (Korea)

    2010-04-15

    Metal oxide-stabilized mesoporous zirconia supports (M-ZrO{sub 2}) with different metal oxide stabilizer (M = Zr, Y, La, Ca, and Mg) were prepared by a templating sol-gel method. 20 wt% Ni catalysts supported on M-ZrO{sub 2} (M = Zr, Y, La, Ca, and Mg) were then prepared by an incipient wetness impregnation method for use in hydrogen production by auto-thermal reforming of ethanol. The effect of metal oxide stabilizer (M = Zr, Y, La, Ca, and Mg) on the catalytic performance of supported nickel catalysts was investigated. Ni/M-ZrO{sub 2} (M = Y, La, Ca, and Mg) catalysts exhibited a higher catalytic performance than Ni/Zr-ZrO{sub 2}, because surface oxygen vacancy of M-ZrO{sub 2} (M = Y, La, Ca, and Mg) and reducibility of Ni/M-ZrO{sub 2} (M = Y, La, Ca, and Mg) were enhanced by the addition of lower valent metal cation. Hydrogen yield over Ni/M-ZrO{sub 2} (M = Zr, Y, La, Ca, and Mg) catalyst was monotonically increased with increasing both surface oxygen vacancy of M-ZrO{sub 2} support and reducibility of Ni/M-ZrO{sub 2} catalyst. Among the catalysts tested, Ni catalyst supported on yttria-stabilized mesoporous zirconia (Ni/Y-ZrO{sub 2}) showed the best catalytic performance. (author)

  18. Germanium nanowires grown using different catalyst metals

    Energy Technology Data Exchange (ETDEWEB)

    Gouveia, R.C., E-mail: riama@ifsp.edu.br [Departamento de Física – NanO Lab, Universidade Federal de São Carlos, Rod. Washington Luís, Km 235 – SP 310, São Carlos, CEP 13565-905 (Brazil); Área de Ciências, Instituto Federal de Educação Ciência e Tecnologia de São Paulo, Rua Américo Ambrósio, 269, Jd. Canaã, Sertãozinho, CEP 14169-263 (Brazil); Kamimura, H.; Munhoz, R.; Rodrigues, A.D. [Departamento de Física – NanO Lab, Universidade Federal de São Carlos, Rod. Washington Luís, Km 235 – SP 310, São Carlos, CEP 13565-905 (Brazil); Leite, E.R. [Departamento de Química – LIEC, Universidade Federal de São Carlos, S