WorldWideScience

Sample records for beta zeolite catalysts

  1. 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.

  2. Rapid synthesis of beta zeolites

    Science.gov (United States)

    Fan, Wei; Chang, Chun -Chih; Dornath, Paul; Wang, Zhuopeng

    2015-08-18

    The invention provides methods for rapidly synthesizing heteroatom containing zeolites including Sn-Beta, Si-Beta, Ti-Beta, Zr-Beta and Fe-Beta. The methods for synthesizing heteroatom zeolites include using well-crystalline zeolite crystals as seeds and using a fluoride-free, caustic medium in a seeded dry-gel conversion method. The Beta zeolite catalysts made by the methods of the invention catalyze both isomerization and dehydration reactions.

  3. ZnO-beta zeolite:As an effective and eco-friendly heterogeneous catalyst for the synthesis of benzothiazole derivatives

    Institute of Scientific and Technical Information of China (English)

    Santosh; S.Katkar; Pravinkumar; H.Mohite; Lakshman; S.Gadekar; Kaluram; N.Vidhate; Machhindra; K.Lande

    2010-01-01

    A cheap and recyclable ZnO-beta zeolite was used as catalyst for the synthesis of benzothiazole derivatives.This method provides several advantages such as environmental friendliness,short reaction times,high yields,simple work-up procedure and catalyst was successfully reused for four cycles without significant loss of activity.

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

    Science.gov (United States)

    Nowicki, Janusz; Mokrzycki, Łukasz; Sulikowski, Bogdan

    2015-04-08

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

  5. Enhanced Activity of Nanocrystalline Beta Zeolite for Acylation of Veratrole with Acetic Anhydride.

    Science.gov (United States)

    Aisha Mahmood Abdulkareem, Al-Turkustani; Selvin, Rosilda

    2016-04-01

    Friedel-Craft acylation of veratrole using homogeneous acid catalysts such as AlCl3, FeCl3, ZnCl2, and HF etc. produces acetoveratrone, (3',4'-dimethoxyacetophenone), which is the intermediate for synthesis of papavarine alkaloids. The problems associated with these homogeneous catalysts can be overcome by using heterogeneous solid catalysts. Since acetoveratrone is a larger molecule, large pore Beta zeolites with smaller particle sizes are beneficial for the liquid-phase acylation of veratrole, for easy diffusion of reactants and products. The present study aims in the acylation of veratrole with acetic anhydride using nanocrystalline Beta Zeolite catalyst. A systematic investigation of the effects of various reaction parameters was done. The catalysts were characterized for their structural features by using XRD, TEM and DLS analyses. The catalytic activity of nanocrystalline Beta zeolite was compared with commercial Beta zeolite for the acylation and was found that nanocrystalline Beta zeolite possessed superior activity.

  6. Catalytic Acylation of Ethylidenecyclohexane over Zeolite Catalysts

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    Some environmentally friendly catalysts such as HY and H-β zeolites,various cation-exchanged β zeolites,and some other solids have been used in the acylation reaction of ethylidenecyclohexane with acetic anhydride at room temperature to synthesize 3-(1-cyclohexenyl)-2-butanone instead of conventional catalysts.The effect of the amount of HY zeolite used on the acylation reaction was investigated.The yield of the acylated product was 72% in the case of n(ethylidenecyclohexane)∶n(acetic anhydride)∶m(HY zeolite)=1 mmol∶10 mmol∶0.100 g,reaction temperature:25 ℃,and reaction time:2 h.The regenerated HY zeolite showed almost the same catalytic activity as the fresh zeolite.

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

    KAUST Repository

    Wang, Jianjian

    2017-03-13

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

  8. Factors affecting drug adsorption on beta zeolites.

    Science.gov (United States)

    Pasti, Luisa; Sarti, Elena; Cavazzini, Alberto; Marchetti, Nicola; Dondi, Francesco; Martucci, Annalisa

    2013-05-01

    The adsorption behaviour of three commonly used drugs, namely ketoprofen, hydrochlorothiazide and atenolol, from diluted aqueous solutions on beta zeolites with different SiO2/Al2O3 ratio (i.e. 25, 38 and 360) was investigated by changing the ionic strength and the pH, before and after thermal treatment of the adsorbents. The selective adsorption of drugs was confirmed by thermogravimetry and X-ray diffraction. The adsorption capacity of beta zeolites was strongly dependent on both the solution pH and the alumina content of the adsorbent. Such a remarkable difference was interpreted as a function of the interactions between drug molecules and zeolite surface functional groups. Atenolol was readily adsorbed on the less hydrophobic zeolite, under pH conditions in which electrostatic interactions were predominant. On the other hand, ketoprofen adsorption was mainly driven by hydrophobic interactions. For undissociated molecules the adsorption capability increased with the increase of hydrophobicity.

  9. Dimerization of norbornene on zeolite catalysts

    Institute of Scientific and Technical Information of China (English)

    N. G. Grigor’eva; S. V. Bubennov; L. M. Khalilov; B. I. Kutepov

    2015-01-01

    The high activity and selectivity of H‐Beta and H‐ZSM‐12 zeolites in the dimerization of norbornene was established. The norbornene conversion reached 100%in chlorinated paraffin and argon gas medium, with a selectivity of dimer formation of 88%–98%. Four stereo‐isomers of the bis‐2,2’‐norbornylidene structure were identified in the dimer fraction, with the (Z)‐anti‐bis‐2,2’‐norbornylidene prevailing over the others.

  10. Polypropylene obtained through zeolite supported catalysts

    Directory of Open Access Journals (Sweden)

    Queli C. Bastos

    2004-01-01

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

  11. Adsorption, Diffusion and Reaction Studies of Hydrocarbons on Zeolite Catalysts

    NARCIS (Netherlands)

    Donk, Sander van

    2002-01-01

    Zeolites are crystalline microporous materials that are widely applied as catalysts in industries like oil refining, basic petrochemistry and fine chemistry. The major benefit of the use of zeolites as catalysts lies in their unique microporous structures. However, in some cases the presence of micr

  12. Mesoporous zeolite single crystal catalysts: Diffusion and catalysis in hierarchical zeolites

    DEFF Research Database (Denmark)

    Christensen, Christina Hviid; Johannsen, Kim; Toernqvist, Eric

    2007-01-01

    During the last years, several new routes to produce zeolites with controlled mesoporosity have appeared. Moreover, an improved catalytic performance of the resulting mesoporous zeolites over conventional zeolites has been demonstrated in several reactions. In most cases, the mesoporous zeolites...... exhibit higher catalytic activity, but in some cases also improved selectivity and longer catalyst lifetime has been reported. The beneficial effects of introducing mesopores into the zeolites has in most instances been attributed to improved mass transport to and from the active sites located...... in the zeolite micropores. Here, we briefly discuss the most important ways of introducing mesopores into zeolites and, for the first time, we show experimentally that the presence of mesopores dramatically increases the rate of diffusion in zeolite catalysts. This is done by studying the elution of iso...

  13. Conversion of rice husk ash to zeolite beta.

    Science.gov (United States)

    Prasetyoko, Didik; Ramli, Zainab; Endud, Salasiah; Hamdan, Halimaton; Sulikowski, Bogdan

    2006-01-01

    White rice husk ash (RHA), an agriculture waste containing crystalline tridymite and alpha-cristobalite, was used as a silica source for zeolite Beta synthesis. The crystallization of zeolite Beta from RHA at 150 degrees C in the presence of tetraethylammonium hydroxide was monitored by XRD, FTIR and (29)Si MAS NMR techniques. It was found that zeolite Beta started to form after 12h and the complete crystallization of zeolite Beta phase was achieved after 2d. XRD, (29)Si MAS NMR and solid yield studies indicate that the transformation mechanism of silica present in RHA to zeolite Beta involves dissolution of the ash, formation of an amorphous aluminosilicate after 6h of crystallization, followed by dissolution in the mother liquor and final transformation to pure zeolite Beta crystals.

  14. Mordenite - Type Zeolite SCR Catalysts with Iron or Copper

    DEFF Research Database (Denmark)

    2012-01-01

    Cu/mordenite catalysts were found to be highly active for the SCR of NO with NH3 and exhibited high resistance to alkali poisoning. Redox and acidic properties of Cu/mordenite were well preserved after poisoning with potassium unlike that of vanadium catalysts. Fe-mordenite catalysts also reveale...... to be essential requirements for the high alkali resistance. Mordenite-type zeolite based catalysts could therefore be attractive alternatives to conventional SCR catalysts for biomass fired power plant flue gas treatment....

  15. Oxidative dehydration of glycerol to acrylic acid over vanadium-impregnated zeolite beta

    Energy Technology Data Exchange (ETDEWEB)

    Pestana, Carolina F.M.; Guerra, Antonio C.O.; Turci, Cassia C. [Universidade Federal do Rio de Janeiro, RJ (Brazil). Inst. de Quimica; Ferreira, Glaucio B. [Universidade Federal Fluminense, Niteroi, RJ (Brazil). Inst. de Quimica; Mota, Claudio J.A., E-mail: cmota@iq.ufrj.br [INCT Energia e Ambiente, Universidade Federal do Rio de Janeiro, RJ (Brazil)

    2013-01-15

    The oxidative dehydration of glycerol to acrylic acid was studied over vanadium-impregnated zeolite Beta. Catalysts were prepared by wet impregnation of ammonium metavanadate over ammonium-exchanged zeolite Beta, followed by air calcination at 823 K. Impregnation reduced the specific surface area, but did not significantly affected the acidity (Bronsted and Lewis) of the zeolites. The catalytic evaluation was carried out in a fixed bed flow reactor using air as the carrier and injecting glycerol by means of a syringe pump. Acrolein was the main product, with acetaldehyde and hydroxy-acetone (acetol) being also formed. Acrylic acid was formed with approximately 25% selectivity at 548 K over the impregnated zeolites. The result can be explained by XPS (X-ray photoelectron spectroscopy) measurements, which indicated a good dispersion of the vanadium inside the pores. (author)

  16. Highly mesoporous single-crystalline zeolite beta synthesized using a nonsurfactant cationic polymer as a dual-function template

    KAUST Repository

    Zhu, Jie

    2014-02-12

    Mesoporous zeolites are useful solid catalysts for conversion of bulky molecules because they offer fast mass transfer along with size and shape selectivity. We report here the successful synthesis of mesoporous aluminosilicate zeolite Beta from a commercial cationic polymer that acts as a dual-function template to generate zeolitic micropores and mesopores simultaneously. This is the first demonstration of a single nonsurfactant polymer acting as such a template. Using high-resolution electron microscopy and tomography, we discovered that the resulting material (Beta-MS) has abundant and highly interconnected mesopores. More importantly, we demonstrated using a three-dimensional electron diffraction technique that each Beta-MS particle is a single crystal, whereas most previously reported mesoporous zeolites are comprised of nanosized zeolitic grains with random orientations. The use of nonsurfactant templates is essential to gaining single-crystalline mesoporous zeolites. The single-crystalline nature endows Beta-MS with better hydrothermal stability compared with surfactant-derived mesoporous zeolite Beta. Beta-MS also exhibited remarkably higher catalytic activity than did conventional zeolite Beta in acid-catalyzed reactions involving large molecules. © 2014 American Chemical Society.

  17. Formulation of cracking catalyst based on zeolite and natural clays

    Energy Technology Data Exchange (ETDEWEB)

    Aliev, R.R.; Lupina, M.I.

    1995-11-01

    Domestically manufactured cracking catalysts are based on a synthetic amorphous aluminosilicate matrix and Y zeolite. A multistage {open_quotes}gel{close_quotes} technology is used in manufacturing the catalysts. The process includes mixing solutions of sodium silicate and acidic aluminum sulfate, forming, syneresis, and activation of the beaded gel. In the manufacture of bead catalysts, the next steps in the process are washing, drying, and calcining; in the manufacture of microbead catalysts, the next steps are dispersion and formation of a hydrogel slurry, spray-drying, and calcining. The Y zeolite is either introduced into the alumina-silica sol in the stage of forming the beads, or introduced in the dispersion stage. With the aim of developing an active and selective cracking catalyst based on Y zeolite and natural clays, with improved physicomechanical properties, the authors carried out a series of studies, obtaining results that are set forth in the present article.

  18. Nonionic emulsion-mediated synthesis of zeolite beta

    Indian Academy of Sciences (India)

    Yuguo Shen; Ying Zhang; Chao Jin; Ying Cao; Wei Gao; Lishan Cui

    2011-07-01

    Zeolite beta synthesis was first carried out in a newly developed emulsion system containing nonionic polyoxyethylated alkylphenol surfactant, which showed interesting non-conventional features. Compared to the conventional hydrothermal synthesis of zeolite beta, the reported nonionic emulsion system showed a faster nucleation rate. Furthermore, the emulsion system could stabilize the beta product and retarded its further transformation to ZSM-5 even under the high crystallization temperature at 453 K. Additionally, the beta particle size could be tuned by the adoption of different lengths of alkyl chain in the surfactant and cosurfactant. Control experiments showed each emulsion component played a crucial role in the zeolite beta growth. The approach proposed in this paper might be extended to apply for the syntheses of other types of zeolites with particle size under control.

  19. Advanced NMR characterization of zeolite catalysts

    Science.gov (United States)

    Welsh, L. B.

    1985-04-01

    The program discussed in this report is a two-year two-phase joint UOP-University of Illinois study of the application of improved high resolution solid state nuclear magnetic resonance (NMR) techniques to the characterization of zeolite catalysts. During the first phase of this program very pure, and in some cases isotopically enriched faujasites will be prepared and studied by magic angle sample spinning NMR (MASS NMR) and variable engine sample spinning NMR (VASS NMR) on 500 and 360 MHz (proton frequency) NMR spectrometers. The NMR techniques that will be emphasized are the measurement and analysis of the (17)O NMR properties, (27)Al NMR intensity quantitation, and (27)Al and (29)Si NMR relaxation rates. During the second phase of this program these NMR techniques will be used to study the effects of impurity concentration, dealumination treatments and cation exchange on the NMR properties of faujasites. The initial emphasis of this program during Phase I is on the preparation and measurement of the NMR properties of (17)O enriched Na-Y faujasties.

  20. Zeolite catalysts and their use in selective catalytic reduction of NOx

    NARCIS (Netherlands)

    Seijger, G.B.F.; Van den Bleek, C.M.; Calis, H.P.A.

    2003-01-01

    The invention is directed to catalyst compositions comprising a zeolite, as well as to processes for the reduction of nitrogen oxides (NOx) employing these catalyst compositions. The catalyst compositions of the invention comprise a zeolite of the ferrierite type (FER), which zeolite is ion exchange

  1. Catalytic transformation of methyl benzenes over zeolite catalysts

    KAUST Repository

    Al-Khattaf, S.

    2011-02-01

    Catalytic transformation of three methyl benzenes (toluene, m-xylene, and 1,2,4-trimethyl benzene) has been investigated over ZSM-5, TNU-9, mordenite and SSZ-33 catalysts in a novel riser simulator at different operating conditions. Catalytic experiments were carried out in the temperature range of 300-400 °C to understand the transformation of these alkyl benzenes over large pore (mordenite and SSZ-33) in contrast to medium-pore (ZSM-5 and TNU-9) zeolite-based catalysts. The effect of reaction conditions on the isomerization to disproportionation product ratio, distribution of trimethylbenzene (TMB) isomers, and p-xylene/o-xylene ratios are reported. The sequence of reactivity of the three alkyl benzenes depends upon the pore structure of zeolites. The zeolite structure controls primarily the diffusion of reactants and products while the acidity of these zeolites is of a secondary importance. In the case of medium pore zeolites, the order of conversion was m-xylene > 1,2,4-TMB > toluene. Over large pore zeolites the order of reactivity was 1,2,4-TMB > m-xylene > toluene for SSZ-33 catalyst, and m-xylene ∼ 1,2,4-TMB > toluene over mordenite. Significant effect of pore size between ZSM-5 and TNU-9 was observed; although TNU-9 is also 3D 10-ring channel system, its slightly larger pores compared with ZSM-5 provide sufficient reaction space to behave like large-pore zeolites in transformation of aromatic hydrocarbons. We have also carried out kinetic studies for these reactions and activation energies for all three reactants over all zeolite catalysts under study have been calculated. © 2011 Elsevier B.V.

  2. Catalytic Transformation of Ethylbenzene over Y-Zeolite-based Catalysts

    KAUST Repository

    Al-Khattaf, Sulaiman

    2008-11-19

    Catalytic transformation of ethylbenzene (EB) has been investigated over ultrastable Y (USY)-zeolite-based catalysts in a novel riser simulator at different operating conditions. The effect of reaction conditions on EB conversion is reported. The USY catalyst (FCC-Y) was modified by steaming to form a significantly lower acidity catalyst (FCC-SY). The current study shows that the FCC-SY catalyst favors EB disproportionation more than cracking. A comparison has been made between the results of EB conversion over the lowly acidic catalyst (FCC-SY) and the highly acidic catalyst (FCC-Y) under identical conditions. It was observed that increase in catalyst acidity favored cracking of EB at the expense of disproportionation. Kinetic parameters for EB disappearance during disproportionation reaction over the FCC-SY catalyst were calculated using the catalyst activity decay function based on time on stream (TOS). © 2008 American Chemical Society.

  3. Catalytic Fast Pyrolysis of Cellulose Using Nano Zeolite and Zeolite/Matrix Catalysts in a GC/Micro-Pyrolyzer.

    Science.gov (United States)

    Lee, Kyong-Hwan

    2016-05-01

    Cellulose, as a model compound of biomass, was catalyzed over zeolite (HY,.HZSM-5) and zeolite/matrix (HY/Clay, HM/Clay) in a GC/micro-pyrolyzer at 500 degrees C, to produce the valuable products. The catalysts used were pure zeolite and zeolite/matrix including 20 wt% matrix content, which were prepared into different particle sizes (average size; 0.1 mm, 1.6 mm) to study the effect of the particle size of the catalyst for the distribution of product yields. Catalytic pyrolysis had much more volatile products as light components and less content of sugars than pyrolysis only. This phenomenon was strongly influenced by the particle size of the catalyst in catalytic fast pyrolysis. Also, in zeolite and zeolite/matrix catalysts the zeolite type gave the dominant impact on the distribution of product yields.

  4. Influence of the aluminium impregnation [ Al(NO33] in the beta zeolite over its acidity

    Directory of Open Access Journals (Sweden)

    Francisco José Sánchez Castellanos

    2010-04-01

    Full Text Available Beta zeolite was impregnated with [ Al(NO33], increasing the aluminium content in increments of 0.05% from 0.00% to 0.25%. A parallel treatment with 0.05% sulphuric acid was also performed; in both cases, methanol was used as solvent (disperse phase. Cation exchange capacity (CEC, ammonia chemisorption, infrared spectroscopy (FIT-IR, scanning electronic microscopy (SEM, X-Ray powder diffraction (XRD, atomic absorption spectroscopy (AAS, titration with sodium hydroxide and nitrogen physisorption at 77K were used to carry out the physical and chemical characterization of the catalysts. Futhermore, the catalysts were employed in the esterification of ethanol with acetic acid, to quantify the effect of aluminium impregnation over the beta zeolite.

  5. Hydrocarbon cracking with yttrium exchanged zeolite y catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Lochow, C.F.; Kovacs, D.B.

    1987-05-12

    A process is described for cracking a gas oil boiling range hydrocarbon feedstock comprising the step of contacting the feedstock in a catalytic cracking zone under catalytic cracking conditions to produce convulsion products comprising gasoline with a catalyst composition. The process comprises: a Y crystalline aluminosilicate zeolite, having the structure of faujasite and having uniform pore diameters and a silica to alumina mole ratio of at least about 5; an inorganic oxide matrix; and the zeolite having been ion exchanged with a mixture of rare earths prior to compositing with the matrix; and the zeolite having been subsequently further ion exchanged with yttrium following compositing with the matrix, whereby the catalyst composition contains 0.30 to 3.0 wt% yttrium.

  6. Tin-containing zeolites are highly active catalysts for the isomerization of glucose in water

    Energy Technology Data Exchange (ETDEWEB)

    Moliner, Manuel [California Inst. of Technology (CalTech), Pasadena, CA (United States); Roman-Leshkov, Yuriy [California Inst. of Technology (CalTech), Pasadena, CA (United States); Davis, Mark E. [California Inst. of Technology (CalTech), Pasadena, CA (United States)

    2010-04-06

    The isomerization of glucose into fructose is a large-scale reaction for the production of high-fructose corn syrup (HFCS; reaction performed by enzyme catalysts) and recently is being considered as an intermediate step in the possible route of biomass to fuels and chemicals. Here, it is shown that a large-pore zeolite that contains tin (Sn-Beta) is able to isomerize glucose to fructose in aqueous media with high activity and selectivity. Specifically, a 10% (wt/wt) glucose solution containing a catalytic amount of Sn-Beta (1:50 Sn:glucose molar ratio) gives product yields of approximately 46% (wt/wt) glucose, 31% (wt/wt) fructose, and 9% (wt/wt) mannose after 30 min and 12 min of reaction at 383 K and 413 K, respectively. This reactivity is achieved also when a 45 wt% glucose solution is used. The properties of the large-pore zeolite greatly influence the reaction behavior because the reaction does not proceed with a medium-pore zeolite, and the isomerization activity is considerably lower when the metal centers are incorporated in ordered mesoporous silica (MCM-41). The Sn-Beta catalyst can be used for multiple cycles, and the reaction stops when the solid is removed, clearly indicating that the catalysis is occurring heterogeneously. Most importantly, the Sn-Beta catalyst is able to perform the isomerization reaction in highly acidic, aqueous environments with equivalent activity and product distribution as in media without added acid. This enables Sn-Beta to couple isomerizations with other acid-catalyzed reactions, including hydrolysis/isomerization or isomerization/dehydration reaction sequences [starch to fructose and glucose to 5-hydroxymethylfurfural (HMF) demonstrated here].

  7. Catalytic Cracking of Palm Oil Over Zeolite Catalysts: Statistical Approach

    Directory of Open Access Journals (Sweden)

    F. A. A. Twaiq and S. Bhatia

    2012-08-01

    Full Text Available The catalytic cracking of palm oil was conducted in a fixed bed micro-reactor over HZSM-5, zeolite ? and ultrastable Y (USY zeolite catalysts. The objective of the present investigation was to study the effect of cracking reaction variables such as temperature, weight hourly space velocity, catalyst pore size and type of palm oil feed of different molecular weight on the conversion, yield of hydrocarbons in gasoline boiling range and BTX aromatics in the organic liquid product.  Statistical Design of Experiment (DOE with 24 full factorial design was used in experimentation at the first stage.  The nonlinear model and Response Surface Methodology (RSM were utilized in the second stage of experimentation to obtain the optimum values of the variables for maximum yields of hydrocarbons in gasoline boiling range and aromatics.  The HZSM-5 showed the best performance amongst the three catalysts tested.  At 623 K and WHSV of 1 h-1, the highest experimental yields of gasoline and aromatics were 28.3 wt.% and 27 wt.%, respectively over the HZSM-5 catalyst.  For the same catalyst, the statistical model predicted that the optimum yield of gasoline was 28.1 wt.% at WHSV of 1.75 h-1 and 623 K.  The predicted optimum yield of gasoline was 25.5 wt.% at 623 K and WHSV of 1 h-1.KEY WORDS: Catalytic Cracking, Palm Oil, Zeolite, Design Of Experiment, Response Surface Methodology.

  8. Spectroscopic and XRD characterisation of zeolite catalysts active for the oxidative methylation of benzene with methane

    Science.gov (United States)

    Adebajo, Moses O.; Long, Mervyn A.; Frost, Ray L.

    2004-03-01

    The benzene methylation with methane over zeolite catalysts was previously shown in our laboratory to require the presence of oxygen. Thus, a two-step mechanism involving the intermediate formation of methanol by partial oxidation of methane followed by the methylation of benzene with methanol in the second step, was postulated. This paper now reports the results of the characterisation of the zeolite catalysts used for the oxidative benzene methylation reaction in order to provide some information about their composition, structure, properties and their behaviour before and after the reaction. The catalysts were characterised by X-ray diffraction (XRD), inductively coupled plasma atomic emission spectroscopy (ICP-AES), X-ray fluorescence (XRF), FT-IR and solid state NMR. XRD results indicate that the crystalline structures of all the ZSM-5 and H-beta catalysts remained unchanged after batch reaction of benzene with methane over the catalysts in agreement with the observation that the catalysts recovered from the reactor could be reused without loss of activity. Elemental analyses and FT-IR data show that as the level of metal ion exchange increases, the Brönsted acid concentration decreases but this metal ion exchange does not totally remove Brönsted acidity. FT-IR results further show that only a small amount of acid sites is actually necessary for a catalyst to be active since used catalysts containing highly reduced Brönsted acidity are found to be reusable without any loss of their activity. 29Si and 27Al magic angle spinning (MAS) NMR together with FT-IR spectra also show that all the active zeolites catalysts contain some extra-framework octahedral aluminium in addition to the normal tetrahedral framework aluminium. The presence of this extra-lattice aluminium does not, however, have any adverse effect on the crystallinity of the catalysts both before and after oxidative benzene methylation reaction. There appears also to be no significant dealumination

  9. Sulfur tolerant zeolite supported platinum catalysts for aromatics hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Bergem, Haakon

    1997-12-31

    The increased demand for transportation fuels at the expence of heavier fuel oil has forced the refinery industry to expand their conversion capacity with hydrotreating as one of the key processes. A shift towards more diesel powered vehicles along with tightening fuel regulations demanding cleaner fuels has lead to increasing interest in catalytic processes for the manufacturing of such environmentally acceptable fuels. This provides the motivation for this thesis. Its main objective was to study possible catalysts active for desulfurization, hydrogenation, and ring-opening of aromatics all in the presence of sulfur. A close examination of the physical properties and kinetical behaviour of the chosen catalysts has been performed. A high pressure reactor setup was designed and built for activity measurements. Zeolite supported platinum catalysts were prepared and both the metal and acid functions were characterized utilizing various experimental techniques. Hydrogenation of toluene was used as a model reaction and the effect of sulfur adsorption on the activity and kinetic behaviour of the catalysts was investigated. The catalyst samples showed hydrogenation activities comparable to a commercial Pt/Al2O3 catalyst. There were no clear differences in the effect of the various sulfur compounds studied. Platinum supported on zeolite Y gave considerably more sulfur tolerant catalysts compared to Al2O3 as support. 155 refs., 58 figs., 36 tabs.

  10. Investigating the Influence of Mesoporosity in Zeolite Beta on its Catalytic Performance for the Conversion of Methanol to Hydrocarbons

    KAUST Repository

    Liu, Zhaohui

    2015-08-26

    Hierarchically porous zeolite Beta (Beta-MS) synthesized by a soft-templating method contains remarkable intra-crystalline mesoporosity, which reduces the diffusion length in zeolite channels down to several nanometers and alters the distribution of Al among distinct crystallographic sites. When used as a catalyst for the conversion of methanol to hydrocarbons (MTH) at 330 oC, Beta-MS exhibited a 2.7-fold larger conversion capacity, a 2.0-fold faster reaction rate, and a remarkably longer lifetime than conventional zeolite Beta (Beta-C). The superior catalytic performance of Beta-MS is attributed to its hierarchical structure, which offers full accessibility to all catalytic active sites. In contrast, Beta-C was easily deactivated because a layer of coke quickly deposited on the outer surfaces of the catalyst crystals, impeding access to interior active sites. This difference is clearly demonstrated by using electron microscopy combined with electron energy loss spectroscopy to probe the distribution of coke in the deactivated catalysts. At both low and high conversions, ranging from 20% to 100%, Beta-MS gave higher selectivity towards higher aliphatics (C4-C7) but lower ethene selectivity compared to Beta-C. Therefore, we conclude that a hierarchical structure decreases the residence time of methylbenzenes in zeolite micropores, disfavoring the propagation of the aromatic-based catalytic cycle. This conclusion is consistent with a recent report on ZSM-5 and is also strongly supported by our analysis of soluble coke species residing in the catalysts. Moreover, we identified an oxygen-containing compound, 4-methyl-benzaldehyde, in the coke, which has not been observed in the MTH reaction before.  

  11. Synthesis H-Zeolite catalyst by impregnation KI/KIO3 and performance test catalyst for biodiesel production

    Science.gov (United States)

    Widayat, W.; Rizky Wicaksono, Adit; Hakim Firdaus, Lukman; Okvitarini, Ndaru

    2016-02-01

    The objective of this research is to produce H-catalyst catalyst that was impregnated with KI/KIO3. The catalyst was analyzed about surface area, X-Ray Diffraction (XRD) and performance test of catalyst for biodiesel production. An H-Zeolite catalyst was synthesized from natural zeolite with chemical treatment processing, impregnation KI/KIO3 and physical treatment. The results shows that the surface area of the catalyst by 27.236 m2/g at a concentration of 5% KI. XRD analysis shows peak 2-θ at 23.627o indicating that KI was impregnated on H-zeolite catalyst. The catalyst was tested in production of biodiesel using palm oil with conventional methods for 3 hour at temperature of 70-80 oC. The result for conversion Fatty Acid Methyl Ester (FAME) reached maximum value on 87.91% under production process using catalyst 5% KIO3-H zeolite.

  12. Fe-BEA Zeolite Catalysts for NH3-SCR of NOx

    DEFF Research Database (Denmark)

    Frey, Anne Mette; Mert, Selcuk; Due-Hansen, Johannes;

    2009-01-01

    Iron-containing zeolites are known to be promising catalysts for the NH3-SCR reaction. Here, we will investigate the catalytic activity of iron-based BEA catalysts, which was found to exhibit improved activities compared to previously described iron-containing zeolite catalysts, such as ZSM-5 and...

  13. Adsorptive desulfurization over hierarchical beta zeolite by alkaline treatment

    Institute of Scientific and Technical Information of China (English)

    Fuping Tian; Xiaojian Yang; Yanchun Shi; Cuiying Jia; Yongying Chen

    2012-01-01

    Hierarchical beta zeolites with SiO2/Al2O3 molar ratios of 16 to 25 were obtained by alkaline treatment in NaOH solution.The effects of treatment temperature on crystallinity,textural properties and chemical composites were studied by XRD,N2 sorption,FT-IR and XRF techniques.The desulfurization performance of parent and alkaline-treated beta zeolites was investigated by static absorption in four model fuels,containing four sulfur compounds of different molecular sizes like thiophene (TP),3-methylthiophene (3-MT),benzothiophene (BT) and dibenzothiophene (DBT),respectively.The crystallinity was observed to be successfully maintained when the treatment temperature was below 50℃.Mesoporosity of beta zeolite was evidently developed with alkaline treatment.The formation of mesopore remarkably improved the desulfurization performance for TP,3-MT,BT and DBT,especially for DBT with larger molecular diameter.Though the addition of toluene in the model fuels resulted in a significant drop of the desulfurization performance of mesoporous beta zeolite,the introduction of cerium ions to some extent mitigated the effect of toluene,which means that both the adsorbents porous structure and the adsorption mode are responsible for the desulfurization performance.The adsorbent of cerium ion-exchanged mesoporous beta showed about 80% recovery of desulfurization after the first regeneration.

  14. Synthesis of mesoporous Beta and Sn-Beta zeolites and their catalytic performances.

    Science.gov (United States)

    Jin, Junjiang; Ye, Xinxin; Li, Yongsheng; Wang, Yanqin; Li, Liang; Gu, Jinlou; Zhao, Wenru; Shi, Jianlin

    2014-06-14

    Mesoporous Beta zeolite has been successfully prepared through hydrothermal synthesis in the presence of cationic ammonium-modified chitosan as the meso-template. Through a subsequent solid-gas reaction between highly dealuminated mesoporous Beta zeolite and SnCl4 steam at an elevated temperature, mesoporous Sn-Beta has been facilely obtained. It was revealed that the addition of cationic chitosan induced the nanocrystal aggregation to particle sizes of ∼300 nm, giving rise to the intercrystalline/interparticle mesoporosity. In the Sn-implanting procedure, Sn species were demonstrated to be doped into the framework of the resulting mesoporous Beta zeolite in a tetrahedral environment without structural collapse. Due to the micro/mesoporous structures, both mesoporous Beta and Sn-Beta exhibited superior performances in α-pinene isomerization, Baeyer-Villiger oxidation of 2-adamantanone by hydrogen peroxide and the isomerization of glucose in water, respectively.

  15. Mesopore quality determines the lifetime of hierarchically structured zeolite catalysts

    Science.gov (United States)

    Milina, Maria; Mitchell, Sharon; Crivelli, Paolo; Cooke, David; Pérez-Ramírez, Javier

    2014-05-01

    Deactivation due to coking limits the lifetime of zeolite catalysts in the production of chemicals and fuels. Superior performance can be achieved through hierarchically structuring the zeolite porosity, yet no relation has been established between the mesopore architecture and the catalyst lifetime. Here we introduce a top-down demetallation strategy to locate mesopores in different regions of MFI-type crystals with identical bulk porous and acidic properties. In contrast, well-established bottom-up strategies as carbon templating and seed silanization fail to yield materials with matching characteristics. Advanced characterization tools capable of accurately discriminating the mesopore size, distribution and connectivity are applied to corroborate the concept of mesopore quality. Positron annihilation lifetime spectroscopy proves powerful to quantify the global connectivity of the intracrystalline pore network, which, as demonstrated in the conversions of methanol or of propanal to hydrocarbons, is closely linked to the lifetime of zeolite catalysts. The findings emphasize the need to aptly tailor hierarchical materials for maximal catalytic advantage.

  16. Fly ash zeolite catalyst support for Fischer-Tropsch synthesis

    Science.gov (United States)

    Campen, Adam

    This dissertation research aimed at evaluating a fly ash zeolite (FAZ) catalyst support for use in heterogeneous catalytic processes. Gas phase Fischer-Tropsch Synthesis (FTS) over a fixed-bed of the prepared catalyst/FAZ support was identified as an appropriate process for evaluation, by comparison with commercial catalyst supports (silica, alumina, and 13X). Fly ash, obtained from the Wabash River Generating Station, was first characterized using XRD, SEM/EDS, particle size, and nitrogen sorption techniques. Then, a parametric study of a two-step alkali fusion/hydrothermal treatment process for converting fly ash to zeolite frameworks was performed by varying the alkali fusion agent, agent:flyash ratio, fusion temperature, fused ash/water solution, aging time, and crystallization time. The optimal conditions for each were determined to be NaOH, 1.4 g NaOH: 1 g fly ash, 550 °C, 200 g/L, 12 hours, and 48 hours. This robust process was applied to the fly ash to obtain a faujasitic zeolite structure with increased crystallinity (40 %) and surface area (434 m2/g). Following the modification of fly ash to FAZ, ion exchange of H+ for Na+ and cobalt incipient wetness impregnation were used to prepare a FTS catalyst. FTS was performed on the catalysts at 250--300 °C, 300 psi, and with a syngas ratio H2:CO = 2. The HFAZ catalyst support loaded with 11 wt% cobalt resulted in a 75 % carbon selectivity for C5 -- C18 hydrocarbons, while methane and carbon dioxide were limited to 13 and 1 %, respectively. Catalyst characterization was performed by XRD, N2 sorption, TPR, and oxygen pulse titration to provide insight to the behavior of each catalyst. Overall, the HFAZ compared well with silica and 13X supports, and far exceeded the performance of the alumina support under the tested conditions. The successful completion of this research could add value to an underutilized waste product of coal combustion, in the form of catalyst supports in heterogeneous catalytic processes.

  17. Catalyst Activity Comparison of Alcohols over Zeolites

    Energy Technology Data Exchange (ETDEWEB)

    Ramasamy, Karthikeyan K.; Wang, Yong

    2013-01-01

    Alcohol transformation to transportation fuel range hydrocarbon on HZSM-5 (SiO2 / Al2O3 = 30) catalyst was studied at 360oC and 300psig. Product distributions and catalyst life were compared using methanol, ethanol, 1-propanol or 1-butanol as a feed. The catalyst life for 1-propanol and 1-butanol was more than double compared to that for methanol and ethanol. For all the alcohols studied, the product distributions (classified to paraffin, olefin, napthene, aromatic and naphthalene compounds) varied with time on stream (TOS). At 24 hours TOS, liquid product from 1-propanol and 1-butanol transformation primarily contains higher olefin compounds. The alcohol transformation process to higher hydrocarbon involves a complex set of reaction pathways such as dehydration, oligomerization, dehydrocyclization, and hydrogenation. Compared to ethylene generated from methanol and ethanol, oligomerization of propylene and butylene has a lower activation energy and can readily take place on weaker acidic sites. On the other hand, dehydrocyclization of propylene and butylene to form the cyclic compounds requires the sits with stronger acid strength. Combination of the above mentioned reasons are the primary reasons for olefin rich product generated in the later stage of the time on stream and for the extended catalyst life time for 1 propanol and 1 butanol compared to methanol and ethanol conversion over HZSM-5.

  18. Removal of organobromine compounds from the pyrolysis oils of flame retarded plastics using zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Hall, William J.; Williams, Paul T. [Energy and Resources Research Institute, University of Leeds, Leeds LS2 9JT (United Kingdom)

    2008-03-15

    Two flame retarded plastics have been pyrolysed in the presence of two zeolite catalysts to remove the organobromine compounds from the derived pyrolysis oil. The flame retarded plastics were, acrylonitrile-butadiene-styrene (ABS) that was flame retarded with tetrabromobisphenol A and high impact polystyrene (HIPS) that was flame retarded with decabromodiphenyl ether. The two catalysts investigated were zeolite ZSM-5 and zeolite Y-Zeolite. Pyrolysis was carried out in a fixed bed reactor at a final pyrolysis temperature of 440 C. The pyrolysis gases were passed immediately to a fixed bed of the catalyst. It was found that the presence of zeolite catalysts increased the amount of gaseous hydrocarbons produced during pyrolysis but decreased the amount of pyrolysis oil produced. In addition, significant quantities of coke were formed on the surface of the catalysts during pyrolysis. The zeolite catalysts were found to reduce the formation of some valuable pyrolysis products such as styrene and cumene, but other products such as naphthalene were formed instead. The zeolite catalysts, especially Y-Zeolite, were found to be very effective at removing volatile organobromine compounds. However, they were less effective at removing antimony bromide from the volatile pyrolysis products, although some antimony bromide was found on the surfaces of the spent catalysts. (author)

  19. Study on Deactivation and Cracking Performance of Catalysts Containing Y and MFI Zeolites

    Institute of Scientific and Technical Information of China (English)

    Chen Zhenyu; Li Caiying; Tian Huiping; Huang Zhiqing

    2004-01-01

    This article investigated the deactivation caused by hydrothermal treatment and metal contamination of two cracking catalysts containing the Y and ZRP- 1 zeolites aimed at maximization of light olefin yield.Test results had shown that the hydrothermal stability and resistance to metal contamination of the ZRP-1zeolite were apparently better than those of the Y zeolite. Hydrothermal treatment and metal contamination had not only changed the catalytic cracking performance of respective zeolites, but at the same time had also modified to a definite degree of the relative proportions of effective components in these two zeolites and affected the synergistic effects between them, resulting in a relative enhancement of secondary cracking ability of the catalyst and increased olefin selectivity in the FCC products. In the course of application of catalyst for maximization of light olefins yield appropriate adjustment of the relative proportion of two active components can help to alleviate the products distribution and selectivity changes caused by deactivationof FCC catalysts.

  20. Alkali resistant Fe-zeolite catalysts for SCR of NO with NH3 in flue gases

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Jensen, Anker Degn; Riisager, Anders

    2011-01-01

    . The effect of potassium doping on the acidic and redox properties of the Fe-zeolite catalysts were studied. The prepared catalysts showed high surface area and surface acidity. This is essential for increased alkali resistivity in comparison with conventional metal oxide supports like, e.g. TiO2 and ZrO2......Fe-zeolite catalysts were prepared by ionexchange and characterized by nitrogen physisorption, electron paramagnetic resonance (EPR) spectroscopy, NH3-temperature programmed desorption (TPD), H2-temperature programmed reduction (TPR) and Energy dispersive X-ray spectroscopy (EDX) methods......, towards e.g. potassium salts in flue gases from biomass fired power plants. These properties allowed both undoped and potassium doped Fe-zeolite catalysts to posses high activity during the selective catalytic reduction (SCR) of NO with NH3. The extent of deactivation of the Fe-zeolite catalysts...

  1. Dimethylether production on zeolite catalysts activated by Cl-, F-and/or ultrasonication

    Institute of Scientific and Technical Information of China (English)

    Sameh M K Aboul-Fotouh; Noha A K Aboul-Gheit; Mona A Naghmash

    2016-01-01

    The chlorinated and fluorinated zeolite catalysts were prepared by the impregnation of zeolites ( H-ZSM-5, H-MOR or H-Y) using two halogen precursors ( ammonium chloride and ammonium fluoride ) in this study. The influence of ultrasonic irradiation was evaluated for optimizing both halogen precursors for production of dimethylether ( DME) via methanol dehydration in a fixed bed reactor. The catalysts were characterized by SEM, XRD, BET and NH3-TPD. The reaction conditions were temperatures from 100 to 300℃ and a WHSV =15. 9 h-1 . All halogenated catalysts show higher catalytic activities at all reaction temperatures studied. However, the halogenated zeolite catalysts prepared under ultrasonic irradiation show higher performance for DME formation. The chlorinated zeolite catalysts show higher activity and selectivity for DME production than the respective fluorinated versions.

  2. A Selective Octane-Enhancing FCC Catalyst Using ZRP Zeolite as an Active Component

    Institute of Scientific and Technical Information of China (English)

    Huang Dayang; Shu Xingtian; He Mingyuan; Yang Xiaoming; Wang Dianzhong; Zong Baoning

    2001-01-01

    A hetero-crystalline seeding method to prepare a unique MFI type zeolite with mesopores of ca. 4 nm diameter designated as the ZRP zeolite, which possesses high stability and selectivity and is used as component of FCC catalysts to produce high-octane gasoline and light olefins, was developed. With the DOCR and DOCP catalysts containing the ZRP zeolite modified by phosphorus-incorporation as the octaneenhancing catalysts, the commercial trial was carried out in a 0.8Mt/a RFCC unit with a feedstock composed of Daqing atmospheric residue. As compared to the base catalyst, the LPG+gasoline+LCO product yield obtained from this catalyst was increased by 0.53m%. Meanwhile, the RON and MON of gasoline was increased by 1.4 and 2.4 units, respectively. The higher increment of MON is attributable to the higher isoparaffines content in gasoline. This result indicates that the ZRP zeolite possesses higher isomerization selectivity.

  3. Production of aromatic hydrocarbons by catalytic pyrolysis of microalgae with zeolites: catalyst screening in a pyroprobe.

    Science.gov (United States)

    Du, Zhenyi; Ma, Xiaochen; Li, Yun; Chen, Paul; Liu, Yuhuan; Lin, Xiangyang; Lei, Hanwu; Ruan, Roger

    2013-07-01

    Catalytic pyrolysis of microalgae and egg whites was investigated to evaluate the performance of different zeolites for the production of aromatic hydrocarbons. Three zeolites with different structures (H-Y, H-Beta and H-ZSM5) were used to study the effect of catalyst type on the aromatic yield. All three catalysts significantly increased the aromatic yields from pyrolysis of microalgae and egg whites compared with non-catalytic runs, and H-ZSM5 was most effective with a yield of 18.13%. Three H-ZSM5 with silica-to-alumina ratios of 30, 80 and 280 were used to study the effect of Si/Al ratio on the aromatic yield. The maximum yield was achieved at the Si/Al ratio of 80, which provides moderate acidity to achieve high aromatic production and reduce coke formation simultaneously. Aromatic production increased with the incorporation of copper or gallium to HZSM-5. However, other studied metals either had no significant influence or led to a lower aromatic yield.

  4. Effect of zeolite catalyst on sugar dehydration for 5-Hydroxymethylfurfural synthesis

    Science.gov (United States)

    Mostapha, Marhaini; Jahar, Noorhasmiera Abu; Chin, Siew Xian; Jaafar, Sharifah Nabihah Syed; Zakaria, Sarani; Aizat, Wan M.; Azizan, Kamalrul Azlan

    2016-11-01

    The effectiveness in the dehydration of sugars into 5-Hydroxymethylfurfural is related to the catalyst existence. A comprehensive synthesis of 5-Hydroxymethylfurfural from fructose, glucose and sucrose (3.73 mmol) with and without addition zeolite catalyst was performed in this study. The reactions were carried out in water-methanol solvent system for 3 hours reaction time at 180°C temperature. The catalytic results from HPLC showed that the reaction with zeolite increases the yield of 5-Hydroxymethylfurfural with 51.72 %, 34.01% and 50.10% for fructose, glucose and sucrose respectively. The study suggests that zeolites promote the isomerization of glucose into fructose to occur and simultaneously catalyze the dehydration of fructose into 5-Hydroxymethylfurfural. Only slight changes on FT-IR spectra of use zeolite after the reaction was observed. Thus suggest that zeolite was a potential catalyst for catalytic reaction for the conversion of sugar into 5-Hydroxymethylfurfural.

  5. Highly Selective Liquid-Phase Benzylation of Anisole with Solid-Acid Zeolite Catalysts

    DEFF Research Database (Denmark)

    Poreddy, Raju; Shunmugavel, Saravanamurugan; Riisager, Anders

    2015-01-01

    Zeolites were evaluated as solid acid catalysts for the liquid-phase benzylation of anisole with benzyl alcohol, benzyl bromide, and benzyl chloride at 80 °C. Among the examined zeolites, H-mordenite-10 (H-MOR-10) demonstrated particular high activity (>99 %) and excellent selectivity (>96...

  6. Nanocrystalline SSZ-39 zeolite as an efficient catalyst for the methanol-to-olefin (MTO) process.

    Science.gov (United States)

    Martín, Nuria; Li, Zhibin; Martínez-Triguero, Joaquín; Yu, Jihong; Moliner, Manuel; Corma, Avelino

    2016-04-26

    The synthesis of nanosized SSZ-39 zeolite has been achieved using a high silica FAU zeolite as the Si and Al source and tetraethylphosphonium (TEP) cations as OSDAs. The obtained SSZ-39 material shows a remarkably high catalyst lifetime compared to conventional SSZ-13 and SSZ-39 materials.

  7. In-situ NMR studies of isobutane activation and exchange in zeolite beta.

    Science.gov (United States)

    Truitt, Matthew J; White, Jeffery L

    2009-04-01

    (1)H solid-state NMR techniques have been used to simultaneously detect the reactivity of both catalyst and alkane reactant protons in an in-situ experimental design. Specifically, the activation of isobutane C-H bonds by the solid acid zeolite H-Beta is directly observed while the reaction is in progress, and the rate of proton transfer between the solid catalyst surface and gaseous isobutane is quantitatively measured using isotopic (1)H/(2)H exchange methods. Arrhenius analysis of isothermal kinetic runs revealed an apparent activation barrier of 70kJ/mole for the exchange process between isobutane and the 12-membered ring H-Beta, which exceeds our previously determined value of 57kJ/mole for isobutane in the 10-membered ring H-ZSM-5 (JACS 2006, v. 128, p. 1848). Estimation of true activation energies using heat of adsorption data from the literature combined with the experimentally measured apparent E(a) suggests that the true activation barrier differs by only 6-7kJ/mole in the two catalysts. We discuss the possibility that subtle shape selectivity, or inverse shape selectivity, and lattice solvation differences between the two catalysts account for the enhanced solvation of the isobutane transition state in HZSM-5 compared to the larger channel H-Beta. In all experiments, the isobutane reagent was treated to eliminate any unsaturated impurities that might serve as initiators for carbenium-ion mechanisms, and the active catalyst was free of any organic contaminants that might serve as a source of unsaturated initiators.

  8. Zeolite ZSM5 catalysts for abatement of nitrogen oxide

    Energy Technology Data Exchange (ETDEWEB)

    Ganemi, Bager

    1999-07-01

    Airborne pollutants from the combustion of fossil fuels are a global problem. Emission of nitrogen oxides (NO{sub x}) is increasing with the worldwide increase in the use of energy. Atmospheric and photochemical reactions link nitrogen oxides to hydrocarbons and tropospheric ozone. The emission of NO{sub x} has to be tackled urgently in order to limit the harmful effects of anthropogenic activity on the environment. The subject of this thesis is catalytic nitrogen oxide abatement through direct decomposition and reduction by methane over ion-exchanged zeolite ZSM5. The work covers catalytic conversion and surface intermediates, including correlations with the level of exchanged Cu{sup 2+} cations and Ni{sup 2+} or Pd{sup 2+} co-cations. Special attention is given to the aluminium content of the support and changes in structural parameters. It was found that NO{sub x} conversion over cation-exchanged ZSM5 is strongly influenced by the ion-exchange procedure and by the above material parameters. Characterization of Cu-ZSM5 reveals that approximately two molecules of water per Cu{sup 2+} ion desorb at temperatures between 150 and 350 Deg C, in addition to the conventional dehydration at lower temperatures. The desorbed water comes from the decomposition of Cu(OH){sub 2}. Decomposition of hydroxylated copper ions results in the formation Of Cu{sup 2+}-O-Cu{sup 2+} dimers, which are suggested to be the active sites for catalytic decomposition of NO. Acid sites are important for the dispersion of copper ions on the catalyst surface. Acid sites are also important for the interaction between copper species and the zeolite. Increased acidity leads to a stronger interaction between the exchanged cation and the framework, i.e. the exchanged cations become more resistant to mobility. The stronger bond between the exchanged cations and lattice oxygen also prevents dealumination of the catalyst and decreases the thermal expansion at higher temperatures. The temperature of

  9. Investigation of the Hydroisomerization Activities of Ni-Mo Catalysts Loaded on HY and HUSY Zeolites

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    A series of Ni-Mo/zeolite-A12O3 catalysts was prepared by incipient wetness impregnation andtheir catalytic experiments were carried out using an automated microflow apparatus. It is concluded that theNi-Mo catalyst loaded on the HUSY has larger BET surface areas and possesses more acid sites than thatloaded on the HY zeolite, and simultaneously the Ni-Mo/HUSY-A12O3 catalyst reveals higher catalytic activ-ity characterized by feedstock conversion and isomer yield which is about two or three times higher than thatof the Ni-Mo/HY-A12O3 catalyst.

  10. Improved Catalysts for Heavy Oil Upgrading Based on Zeolite Y Nanoparticles Encapsulated Stable Nanoporous Host

    Energy Technology Data Exchange (ETDEWEB)

    Conrad Ingram; Mark Mitchell

    2007-09-30

    The objective of this project is to synthesize nanocrystals of highly acidic zeolite Y nanoclusters, encapsulate them within the channels of mesoporous (nanoporous) silicates or nanoporous organosilicates, and evaluate the 'zeolite Y/Nanoporous host' composites as catalysts for the upgrading of heavy petroleum feedstocks. In comparison to conventionally-used zeolite Y catalysts of micron size particles, the nanocrystals (< 100 nm particle size) which contain shorter path lengths, are expected to allow faster diffusion of large hydrocarbon substrates and the catalysis products within and out of the zeolite's channels and cages (<1 nm size). This is expected to significantly reduce deactivation of the catalyst and to prolong their period of reactivity. Encapsulating zeolite Y nanocrystals within the nanoporous materials is expected to protect its external surfaces and pore entrances from being blocked by large hydrocarbon substrates, since these substrates will initially be converted to small molecules by the nanoporous host (a catalyst in its own right). The project consisted of four major tasks as follows: (1) synthesis of the nanoparticles of zeolite Y (of various chemical compositions) using various techniques such as the addition of organic additives to conventional zeolite Y synthesis mixtures to suppress zeolite Y crystal growth; (2) synthesis of nanoporous silicate host materials of up to 30 nm pore diameter, using poly (alkylene oxide) copolymers which when removed will yield a mesoporous material; (3) synthesis of zeolite Y/Nanoporous Host composite materials as potential catalysts; and (4) evaluation of the catalyst for the upgrading of heavy petroleum feedstocks.

  11. Development of advanced zeolite catalysts for the vapor phase Beckmann rearrangement of cyclohexanone oxime

    Science.gov (United States)

    Dai, Lian-Xin; Iwaki, Yoshihide; Koyama, Katsuyuki; Tatsumi, Takashi

    1997-11-01

    The vapor phase Beckmann rearrangement of cyclohexanone oxime to ɛ-caprolactam catalyzed by various zeolites was studied. The catalytic performance was greatly affected by both the zeolite structure and diluent solvent. When 1-hexanol was used in place of benzene, the catalytic performance of all catalysts except silicalite-1 was greatly improved. In particular, the selectivity and stability of H-LTL and H-OFF-ERI zeolites remarkably increased; both catalysts exhibited ca. 100% oxime conversion and ɛ-caprolactam selectivity of >95% for 6 h.

  12. In Situ Spectroscopic Studies of Proton Transport in Zeolite Catalysts for NH3-SCR

    Directory of Open Access Journals (Sweden)

    Peirong Chen

    2016-12-01

    Full Text Available Proton transport is an elementary process in the selective catalytic reduction of nitrogen oxides by ammonia (DeNOx by NH3-SCR using metal-exchanged zeolites as catalysts. This review summarizes recent advancements in the study of proton transport in zeolite catalysts using in situ electrical impedance spectroscopy (IS under NH3-SCR reaction conditions. Different factors, such as the metal cation type, metal exchange level, zeolite framework type, or formation of intermediates, were found to influence the proton transport properties of zeolite NH3-SCR catalysts. A combination of IS with diffuse reflection infrared Fourier transformation spectroscopy in situ (in situ IS-DRIFTS allowed to achieve a molecular understanding of the proton transport processes. Several mechanistic aspects, such as the NH3-zeolite interaction, NO-zeolite interaction in the presence of adsorbed NH3, or formation of NH4+ intermediates, have been revealed. These achievements indicate that IS-based in situ methods as complementary tools for conventional techniques (e.g., in situ X-ray absorption spectroscopy are able to provide new perspectives for the understanding of NH3-SCR on zeolite catalysts.

  13. Characterization and Design of Zeolite Catalysts Solid Acidity, Shape Selectivity and Loading Properties

    CERN Document Server

    Niwa, Miki; Okumura, Kazu

    2010-01-01

    Zeolites are microporous, aluminosilicate minerals commonly used as commercial adsorbents. Zeolite-based catalysts are used by industrial chemical companies in the interconversion of hydrocarbons and the alkylation of aromatic compounds. The current book deals with the characterization of specific properties of Zeolites and calculations for the design of catalysts. Measurements and utilization of solid acidity, shape selectivity, and loading properties, that are three prominent properties of a Zeolite catalyst, are treated in detail. These features concern chemical vapor deposition of silica, shape selectivity, loading properties, solid activity, Brønsted or Lewis character, ammonia temperature programmed desorption, control of the pore-opening size by chemical vapor deposition of silica and XAFS analysis of metals being highly dispersed inside and outside a framework.

  14. Transalkylation of Multi-secbutylbenzenes with Benzene over Hierarchical Beta Zeolite

    Institute of Scientific and Technical Information of China (English)

    Yingxia Li; Can Luo; Xuan Wang; Chongpin Huang; Biaohua Chen

    2014-01-01

    A hierarchical beta zeolite synthesized by quasi-solid phase conversion method was characterized by BET, scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray diffraction (XRD), temperature-programmed desorption of ammonia (NH3-TPD), 27Al and 29Si magic angle spinning nuclear magnetic resonance (27Al and 29Si MAS NMR), and its catalytic performance was compared with that of conventional microporous beta zeolite for liquid phase transalkylation of multi-secbutylbenzenes (MSBBs) with benzene. The results indicate that the hierarchical beta zeolite consists of nanosized crystals with a meso/microporous structure and has stronger acid strength than the microporous beta zeolite. The higher conversion of tri-secbutylbenzene (TSBB) and selectivity of sec-butylbenzene (SBB) are achieved on hierarchical beta zeolite than microporous beta zeolite, while the conversion of di-secbutylbenzene (DSBB) is slightly higher. The improvement of catalytic performance over hierarchical beta zeolite can be ascribed to the presence of mesopores, nanosized crystals and stronger acidity.

  15. Anticorrosion Nanocrystalline Beta Zeolite Thin Film for Advanced Applications

    Directory of Open Access Journals (Sweden)

    Maha Saud M. Al-subaie

    2015-01-01

    Full Text Available Steel alloys corrosion is ubiquitous and is conventionally protected by anticorrosion chromate coatings. However, the process suffers from the release of carcinogenic hexavalent chromium ions that needs to be replaced by an ecofriendly alternative. In this context, the need for the development of satisfactory ecofriendly chromium-free coating with superior corrosion performance is highly desirable. In the present study, we synthesized fully dispersible nanocrystalline Beta zeolite seeds and coated on steel alloys followed by steaming. The samples were characterized by XRD, FE-SEM, and DLS analyses. The anticorrosion behavior of the synthesized nanoparticle coatings on steel alloys was investigated by electrochemical measurements (DC polarization and electrochemical impedance spectroscopy (EIS in NaCl and acid and alkaline media under identical experimental conditions. The present study demonstrated that the nanozeolite coating can be a potential alternative for toxic and carcinogenic chromate coating.

  16. Effect of the formation of secondary pores in zeolite ZSM-5 on the properties of molybdenum-zeolite catalysts for methane aromatization

    Science.gov (United States)

    Kucherov, A. V.

    2014-03-01

    A study is performed of 4% Mo/ZSM-5 (30) catalysts for methane aromatization prepared by solid-phase synthesis with mechanical mixing of a zeolite with MoO3 followed by calcination at 550°C. Zeolite etched with sodium hydroxide solutions and dealuminated with aluminum nitrate solutions is used as a support. Catalytic studies of the catalysts are conducted. The effect of treating the initial zeolite on the properties of catalysts in methane aromatization is determined. The effect subsequently treating a zeolite support has on the acid sites of a catalyst is confirmed by means of temperature-programmed reduction and the temperature-programmed desorption of NH3. The formation of molybdenum ions in the +5 oxidation state during catalysis and the presence of graphitized carbon deposits on a spent catalyst's surface are confirmed by EPR and temperature-programmed oxidation.

  17. Palladium-Zeolite nanofiber as an effective recyclable catalyst membrane for water treatment.

    Science.gov (United States)

    Choi, Jungsu; Chan, Sophia; Yip, Garriott; Joo, Hyunjong; Yang, Heejae; Ko, Frank K

    2016-09-15

    Zeolite is an exciting natural material due to its unique capability of ammonium nitrogen (NH3N) adsorption in water. In this study, multifunctional hybrid composites of zeolite/palladium (Ze/Pd) on polymer nanofiber membranes were fabricated and explored for sustainable contaminant removal. SEM and XRD demonstrated that zeolite and palladium nanoparticles were uniformly distributed and deposited on the nanofibers. NH3N recovery rate was increased from 23 to 92% when palladium coated zeolite was embedded on the nanofiber. Multifunctional nanofibers of Ze/Pd membranes were able to adsorb NH3N on the zeolites placed on the surface of fibers and palladium catalysts were capable of selective oxidation of NH3N to N2 gas. The cycling of NH3N adsorption-oxidation, high flux, hydrophilicity, and flexibility of the membrane makes it a strong candidate for water treatment.

  18. Design of effective zeolite catalysts for the complete hydrogenation of CO2.

    Science.gov (United States)

    Chan, Bun; Radom, Leo

    2006-04-26

    Ab initio molecular orbital calculations have been applied to the study of the three-stage zeolite-catalyzed hydrogenation of CO2 to methanol. The results present strong evidence that appropriate chemical modifications to ZSM-5 can lead to significantly lower energy barriers for the three component reactions, that is, hydrogenation of CO2, HCO2H, and CH2O. Zeolites incorporating either Na+ or Ge are more effective catalysts than conventional acidic zeolites for the hydrogenation of CO2 to give HCO2H, but amine-based zeolites do not lead to significantly lower barriers for any of the three hydrogenation reactions. However, we predict that when all three features, namely, Na+, N, and Ge, are incorporated in the zeolite, there is a dramatic improvement in catalytic activity for all three reactions.

  19. Local Environment and Nature of Cu Active Sites in Zeolite-Based Catalysts for the Selective Catalytic Reduction of NOx

    NARCIS (Netherlands)

    Deka, U.; Lezcano-Gonzalez, I.; Weckhuysen, B.M.; Beale, A.M.

    2013-01-01

    Cu-exchanged zeolites have demonstrated widespread use as catalyst materials in the abatement of NOx, especially from mobile sources. Recent studies focusing on Cu-exchanged zeolites with the CHA structure have demonstrated them to be excellent catalysts in the ammonia-assisted selective catalytic r

  20. Alkali resistant Cu/zeolite deNOx catalysts for flue gas cleaning in biomass fired applications

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Riisager, Anders; Fehrmann, Rasmus

    2011-01-01

    Cu/zeolite catalysts have been prepared by wet impregnation and characterized by N2 physisorption, EPR, H2-TPR and NH3-TPD methods. The Cu content was varied to optimize the loading as well as surface acidity. Optimized Cu/zeolite catalysts showed high surface acidity and excellent activity...

  1. Dealuminated ZSM—5 Zeolite Catalyst for Ethylene Oligomerization to Liquid Fuels

    Institute of Scientific and Technical Information of China (English)

    NorAishahSaidinaAmin; DidiDwiAnggoro

    2002-01-01

    Ethylene oligomerization using ZSM-5 zeolite was investigated to study the role of Broensted acid sites in the formation of higher hydrocarbons,The oligomeriztion of olefins,dependent on the acidity of ZSM-5 zeolite ,is an important step in the conversion of natural gas to liquied fuels,The framework Si/Al ratio reflects the number of potential acid sites and the acid strength of the ZSM-5 catalyst,ZSM-5 with the mole ratio SiO2/Al2O3 equal to 30 was dealuminated for different periods of time according to the acidic ion-exchange method to produce ZSM-5 with various Si/Al ratios,The FT-IR analysis revealed that the integrated framework aluminum band,non-framework aluminum band,and silanol groups areas of the ZSM-5 zeolites decreased after being dealuminated,The performanc of the dealuminated zeolite was tested for ethylene oligomerization.The results demonstrated that the dealumination of ZSM-5 led to higher ethylene conversion,but the gasoline selectivity was reduced compared to the performance of a ZSM-5 zeolite ,The characterization results revealed the amount of aluminum in the zeolitic framework,the crystallinity of the ZSM-5 zeolite,and the Si/Al ration affected the formation of Broensted acid sites,The number of the Broensted acid sites on the catalyst active sites is important in the olefin conversion to liquied hydrocarbons.

  2. 3D Nanoscale Imaging and Quantitative Analysis of Zeolite Catalysts

    NARCIS (Netherlands)

    Zecevic, J.

    2013-01-01

    Zeolites are crystalline microporous aluminosilicates, one of the most versatile and widely used class of materials.The unique physico-chemical properties of zeolites are found to be irreplaceable in many industrial processes such as separation, adsorption and catalysis. To exploit their full potent

  3. Hydrocarbon cracking selectivities with a dual zeolite fluid cracking catalyst containing REY and ZSM-5

    Energy Technology Data Exchange (ETDEWEB)

    Rajagopalan, K.; Young, G.W. (W.R. Grace and Company, Columbia, MD (USA))

    1987-08-01

    Synthetic Y faujasite zeolites have been used commercially as cracking catalysts for the past two decades, and more recently dual zeolite fluid cracking catalysts, containing faujasite and ZSM-5 were discovered to increase the octane number of the gasoline during catalytic cracking of gas oil. This concept, where ZSM-5 constitutes only a small fraction (about 1 wt %) of the cracking catalyst, has been tested commercially in Europe and in the United States. Cracking of paraffinic and olefinic hydrocarbons by ZSM-5 catalysts has been studied by several investigators over a range of temperatures (350 to 540{degree}C) and using nearly pure ZSM-5 as the catalyst. The mechanism of octane number enhancement with the dual zeolite catalyst was investigated by examining the effect on product selectivity of addition of 1 wt % ZSM-5 to a cracking catalyst composition during catalytic cracking of a commercial gas oil at 500{degree}C. Changes in composition of the product gasoline (paraffins, olefins, naphthenes and aromatics) caused by ZSM-5 were measured. Since commercial cracking catalysts undergo continuous high temperature regeneration in the presence of steam, the effect of hydrothermal treatment of ZSM-5 was also investigated.

  4. Physico-chemical Characterization of Mo-Hβ Zeolite Catalysts

    Institute of Scientific and Technical Information of China (English)

    LIU Sheng-lin; HUANG Sheng-jun; XIN Wen-jie; QIN xin-hua; XIE Su-juan; XU Long-ya

    2004-01-01

    A series of Mo-impregnated Hβ samples, with MoO3 loading in Hβ zeolite in the mass fraction range of 0. 5%-6.0%, were studied by means of XRD and IR in order to characterize their structures. Mo/Hβ samples' crystallinity almost linearly decreases with increasing the amount of MoO3 loaded. The IR spectra and XRD patterns suggest that the progressive destabilization of the Hβ zeolite structure is caused by increasing Mo loading in (MoO3+Hβ zeolite). During the calcination, Al2(MoO4)3 formed from the dealumination of Hβ zeolite, causes the substantially partial breakdown of the zeolite framework when the Mo loading in MoO3 +Hβ is relatively high.

  5. Conversion of bio-feedstocks through acid and basic zeolites and catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Buzzoni, R.; Bosetti, A.; Delledonne, D.; Perego, C. [eni S.p.A. Research Centre for Non-Conventional Energy, Novara (Italy). Ist. eni Donegani

    2012-07-01

    Not far in the future, a significant part of fuels and chemicals will be originated by renewable biomass resources. In this respect, zeolite catalysts may help to develop a new generation of bio-fuel and chemical processes. In the new bio-paradigm not only acid but also basic materials will have an important and dominant role. Just to give some examples, basic zeolites based catalysts have been proposed for transesterification of triglyceride esters of fatty acids to biodiesel, for disrupting the lignin polymer by base catalyzed depolymerisation and for one pot lignin liquefaction by hydrogenation. (orig.)

  6. Preparation and Characterization of Zeolite Beta with Low SiO2/Al2O3 Ratio

    Institute of Scientific and Technical Information of China (English)

    Kang Shanjiao; Gong Yanjun; Dou Tao; Zhang Ying; Zheng Yanying

    2007-01-01

    Zeolite beta with a low SiO2/Al2O3 ratio was synthesized by a novel two-step process. The synthesized sample was characterized with XRD,SEM,FTIR,and N2 adsorption-desorption and solid-state MAS NMR. The results showed that aluminium species were inserted into the framework of zeolite beta. The BET surface area,volume,and particle size of the zeolite beta sample decreased with decreasing SiO2/Al2O3 ratio. Our process was proved an efficient route to synthesize zeolite beta with a low SiO2/Al2O3 ratio.

  7. Dealuminated ZSM-5 Zeolite Catalyst for Ethylene Oligomerization to Liquid Fuels

    Institute of Scientific and Technical Information of China (English)

    Nor Aishah Saidina Amin; Didi Dwi Anggoro

    2002-01-01

    Ethylene oligomerization using ZSM-5 zeolite was investigated to study the role of Bronstedacid sites in the formation of higher hydrocarbons. The oligomerization of olefins, dependent on the acidityof ZSM-5 zeolite, is an important step in the conversion of natural gas to liquid fuels. The framework Si/Alratio reflects the number of potential acid sites and the acid strength of the ZSM-5 catalyst. ZSM-5 withthe mole ratio SiO2/Al2O3 equal to 30 was dealuminated for different periods of time according to theacidic ion-exchange method to produce ZSM-5 with various Si/Al ratios. The FT-IR analysis revealedthat the integrated framework aluminum band, non-framework aluminum band, and silanol groups areasof the ZSM-5 zeolites decreased after being dealuminated. The performance of the dealuminated zeolitewas tested for ethylene oligomerization. The results demonstrated that the dealumination of ZSM-5 ledto higher ethylene conversion, but the gasoline selectivity was reduced compared to the performance of aZSM-5 zeolite. The characterization results revealed the amount of aluminum in the zeolitic framework,the crystallinity of the ZSM-5 zeolite, and the Si/Al ratio affected the formation of Bronsted acid sites.The number of the Bronsted acid sites on the catalyst active sites is important in the olefin conversion toliquid hydrocarbons.

  8. Zeolite-based SCR catalysts and their use in diesel engine emission treatment

    Energy Technology Data Exchange (ETDEWEB)

    Narula, Chaitanya K.; Yang, Xiaofan

    2016-08-02

    A catalyst comprising a zeolite loaded with copper ions and at least one trivalent metal ion other than Al.sup.+3, wherein the catalyst decreases NO.sub.x emissions in diesel exhaust. The trivalent metal ions are selected from, for example, trivalent transition metal ions, trivalent main group metal ions, and/or trivalent lanthanide metal ions. In particular embodiments, the catalysts are selected from Cu--Fe-ZSM5, Cu--La-ZSM-5, Fe--Cu--La-ZSM5, Cu--Sc-ZSM-5, and Cu--In-ZSM5. The catalysts are placed on refractory support materials and incorporated into catalytic converters.

  9. Zeolite-based SCR catalysts and their use in diesel engine emission treatment

    Science.gov (United States)

    Narula, Chaitanya K; Yang, Xiaofan

    2015-03-24

    A catalyst comprising a zeolite loaded with copper ions and at least one trivalent metal ion other than Al.sup.+3, wherein the catalyst decreases NO.sub.x emissions in diesel exhaust. The trivalent metal ions are selected from, for example, trivalent transition metal ions, trivalent main group metal ions, and/or trivalent lanthanide metal ions. In particular embodiments, the catalysts are selected from Cu--Fe-ZSM5, Cu--La-ZSM-5, Fe--Cu--La-ZSM5, Cu--Sc-ZSM-5, and Cu--In-ZSM5. The catalysts are placed on refractory support materials and incorporated into catalytic converters.

  10. Synthesis of isoalkanes over a core (Fe-Zn-Zr)-shell (zeolite) catalyst by CO2 hydrogenation.

    Science.gov (United States)

    Wang, Xiaoxing; Yang, Guohui; Zhang, Junfeng; Chen, Shuyao; Wu, Yingquan; Zhang, Qingde; Wang, Junwei; Han, Yizhuo; Tan, Yisheng

    2016-05-31

    A kind of core-shell catalyst with Fe-Zn-Zr as the core and a zeolite (HZSM-5, Hbeta, and HY) as the shell was synthesized by a simple cladding method. The catalyst has an obvious confinement effect on the synthesis of isoalkanes by CO2 hydrogenation. Especially, the Fe-Zn-Zr@HZSM-5-Hbeta catalyst with a double-zeolite shell exhibits an extraordinary high i-HC/t-HC ratio.

  11. Study on Aromatization of C6 Aliphatic Hydrocarbons on ZRP Zeolite Catalyst

    Institute of Scientific and Technical Information of China (English)

    Wang Yongjun; Xie Chaogang

    2004-01-01

    The performance of ZRP zeolite catalysts for aromatization of C6 aliphatic hydrocarbons was investigated in a pulsed microreactor. The influence of metal modified ZRP zeolites on aromatization reaction was also studied, coupled with comparison of aromatization tendencies of olefins, paraffins and paraffins with different degrees of chain branching. Test results had shown that the lower the silicon/aluminum ratio in the ZRP zeolite, the higher the aromatization reactivity of aliphatic hydrocarbons. Modification of ZRP zeolite by zinc and its zinc content had apparent impact on the yield and distribution of aromatics. The aromatization tendency of olefins was apparently better than paraffins, while the aromatization tendency of monomethyl paraffins was better than that of straight-chain paraffins with the exception of dimethyl paraffins, which had worse aromatization tendency because of their steric hindrance.

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

    OpenAIRE

    F. V. Barsi; Cardoso,D.

    2009-01-01

    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 th...

  13. Evaluation of photocatalytic activities of supported catalysts on NaX zeolite or activated charcoal.

    Science.gov (United States)

    de Brites-Nóbrega, Fernanda F; Polo, Aldino N B; Benedetti, Angélica M; Leão, Mônica M D; Slusarski-Santana, Veronice; Fernandes-Machado, Nádia R C

    2013-12-15

    This study aimed to evaluate the photocatalytic activity of ZnO and Nb2O5 catalysts, both supported on NaX zeolite and activated charcoal (AC). The synergistic effect between oxide and support and the influence of solution pH (3, 7 and 9) on photocatalytic degradation of reactive blue 5G (C.I. 222) were analyzed. The catalysts Nb2O5/NaX, Nb2O5/AC and ZnO/NaX, ZnO/AC with 5 and 10% (wt%) were prepared by wet impregnation. The results showed that the catalysts exhibit quite different structural and textural properties. The synergic effect between ZnO and NaX support was higher than that with the activated charcoal, showing that these catalysts were more efficient. The most photoactive catalyst was 10% ZnO/NaX which showed 100% discoloration of the dye solution at pH 3, 7 and 9 after 0.5, 5 and 2h of irradiation, respectively. The hydrolytic nature of zeolite favored the formation of surface hydroxyl radicals, which increased the activity of the photocatalyst. Thus, catalysts supported on NaX zeolite are promising for use in photocatalysis.

  14. Selective preparation of zeolite X and A from flyash and its use as catalyst for biodiesel production

    Energy Technology Data Exchange (ETDEWEB)

    Volli, Vikranth; Purkait, M.K., E-mail: mihir@iitg.ernet.in

    2015-10-30

    Highlights: • Flyash was utilized for zeolites preparation for transesterification. • Single phase and highly crystalline zeolite was obtained at flyash/NaOH ratio of 1:1.2. • Si/Al ratio of 2 resulted in the formation of zeolite X. • At 5 wt% of catalyst loading conversion was 84.6%. • The biodiesel obtained has a calorific value of 37.5 MJ/Kg. - Abstract: This work discusses the utilization of flyash for synthesis of heterogeneous catalyst for transesterification. Different types of zeolites were synthesized from alkali fusion followed by hydrothermal treatment of coal flyash as source material. The synthesis conditions were optimized to obtain highly crystalline zeolite based on degree of crystallinity and cation exchange capacity (CEC). The effect of CEC, acid treatment, Si/Al ratio and calcination temperature (800, 900 and 1000 °C) on zeolite formation was also studied. Pure, single phase and highly crystalline zeolite was obtained at flyash/NaOH ratio (1:1.2), fusion temperature (550 °C), fusion time (1 h), hydrothermal temperature (110 °C) and hydrothermal time (12 h). The synthesized zeolite was ion-exchanged with potassium and was used as catalyst for transesterification of mustard oil to obtain a maximum conversion of 84.6% with 5 wt% catalyst concentration, 12:1 methanol to oil molar ratio, reaction time of 7 h at 65 °C. The catalyst was reused for 3 times with marginal reduction in activity.

  15. Zeolite-supported precious metal catalysts for NO{sub x} reduction in lean burn engine exhaust

    Energy Technology Data Exchange (ETDEWEB)

    Takami, A.; Takemoto, T.; Iwakuni, H.; Yamada, K.; Shigetsu, M.; Komatsu, K. [Technical Research Center, Mazda Motor Corporation, Hiroshima (Japan)

    1997-03-06

    The effects of the zeolite-supported precious metal catalysts on NO{sub x} reduction in oxygen-rich exhaust have been investigated. It became clear that NO{sub x} conversion related the number of NO adsorption sites of precious metal and the number of HC (C{sub 3}H{sub 6}) adsorption of support (zeolite). Pt-Ir-Rh/MFI zeolite catalyst showed higher performance and durability than the current Pt-Rh supported on alumina and ceria catalyst

  16. Removal of flotation reagents from process water by adsorption onto spent zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Oliveira, J.F.; Valdiviezo, E. [COPPE/UFRJ, Rio de Janeiro (Brazil). Dept. of Materials and Metallurgical Engineering]|[CETEM/CNPQ, Rio de Janeiro (Brazil). Center for Mineral Technology

    1995-12-31

    Adsorption of residual flotation reagents onto equilibrium fluid cracking catalysts is a promising method of purification of flotation process water. In the present paper, adsorption of sodium dodecyl sulfate (SDS), dodecyl ammonium chloride (DAC) and sodium oleate onto a spent catalyst from petroleum industry was studied by analyzing the residual concentration of the surfactant after contact with the zeolite catalyst. The adsorption of the DAC was rather low but SDS and sodium oleate presented a high affinity for the catalyst surface. The loading capacity was 4.2 kg/ton for SDS and 5.5 kg/ton for oleic acid. After the treatment of the loaded catalyst with a HCl 1N solution these surfactants are desorbed and the catalyst may thus be regenerated. This would be an additional advantage to its low cost, not to mention its condition as a discarded product and its availability in large tonnages.

  17. Mesoporous zeolite SBA-15 supported nickel diimine catalysts for ethylene polymerization

    Institute of Scientific and Technical Information of China (English)

    GUO Chao; ZHANG Dao; JIN Guoxin

    2004-01-01

    The novel mesoporous zeolite SBA-15 is successfully used as the support to immobilize late-transition metal nickel diimine catalyst, both in physical and chemical methods, EA, ICP, FT-IR and XRD are applied to characterizing these supported catalysts. The results of ethylene polymerization reveal that these supported catalysts have high catalytic activity as their homogenous counterpart does, moreover, polyethylene with a fibrous morphology is produced due to the channel effect of support, and both the molecular weight and molecular weight distributions of polymers are increased greatly.

  18. THE OPTIMIZATION OF PRODUCTION ZEOLITE Y CATALYST FROM RHA BY RESPONSE SURFACE METHODOLOGY

    Directory of Open Access Journals (Sweden)

    Didi Dwi Anggoro

    2012-02-01

    Full Text Available Rice husk is the milling byproduct of rice and is a major waste product of the agriculture industry. Amorphous silica, commonly referred to as rice husk ash, was extracted from rice husk by acid leaching, pyrolysis, and carbon-removing processes. These properties make the ash a valuable raw material for many industries.  This paper is study of synthesized of zeolite Y from rice husk ash. Zeolite Y synthesis is used for petroleum industry as expensive catalyst. Rice husk was calcined at temperature 700oC for two hours using furnace to produce pure silica. The composition of synthesized of zeolite Y from rice husk was 2.24 Na2O:Al2O3:8SiO2:112 H2O. The gel solution was mixed at room temperature for 24 hours using autoclave. Then, the gel solution was heated with variable temperature and time crystallization. The product zeolite synthesis Y was filtered and washed with distilled water until pH lower than ten, than dried at oven. This product was analyzed with X-Ray Diffraction (XRD. From XRD analyze result indicated that from rice husk ash can produced zeolite synthesis Y which high crystallization degree. The optimum conditions for synthesis of zeolite Y from rice husk ash are temperature at 100oC for 48 hours, silicate at 20%, and aluminate at 10%.

  19. THE OPTIMIZATION OF PRODUCTION ZEOLITE Y CATALYST FROM RHA BY RESPONSE SURFACE METHODOLOGY

    OpenAIRE

    Didi Dwi Anggoro; Aprilina Purbasari

    2012-01-01

    Rice husk is the milling byproduct of rice and is a major waste product of the agriculture industry. Amorphous silica, commonly referred to as rice husk ash, was extracted from rice husk by acid leaching, pyrolysis, and carbon-removing processes. These properties make the ash a valuable raw material for many industries.  This paper is study of synthesized of zeolite Y from rice husk ash. Zeolite Y synthesis is used for petroleum industry as expensive catalyst. Rice husk was calcined at t...

  20. Mechanism of reaction of phenol with toluene on a zeolite catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Kozhevnikov, S.A.; Sibarov, D.A.; Proskuryakov, V.A.

    1988-04-10

    The high-molecular-weight products formed from phenol and toluene on zeolite-containing catalyst were isolated and studied. By independent synthesis, and by PMR, /sup 13/C NMR, IR, and TLC methods it was shown that these products are hydroxy- and dihydroxydiphenyl-methane type compounds. The role of hydroxy- and dihydroxydiphenylmethanes as intermediates in cresol formation from phenol and toluene and their high coking activity were proved. A probable mechanism of cresol formation was proposed with the participation of hydroxy- and dihydroxydiphenylmethanes in the reaction of phenol with toluene on zeolites.

  1. Improved Catalysts for Heavy Oil Upgrading Based on Zeolite Y Nanoparticles Encapsulated Stable Nanoporous Host

    Energy Technology Data Exchange (ETDEWEB)

    Conrad Ingram; Mark Mitchell

    2006-09-30

    The addition of hydrothermally-aged zeolite Y precursor to an SBA-15 synthesis mixture under a mildly acidic condition resulted in the formation of mesoporous aluminosilicate catalyst, Al-SBA-15, containing strong Broensted acid sites and aluminum (Al) stabilized in a totally tetrahedral coordination. The physicochemical characteristics of the catalyst varied as a function of the synthesis conditions. The catalyst possessed surface areas ranging between 690 and 850 m{sup 2}/g, pore sizes ranging from 5.6 to 7.5 nm, and pore volumes up 1.03 cm{sup 3}, which were comparable to the parent SBA-15 synthesized under similar conditions. Two wt% Al was present in the catalyst that was obtained from the reaction mixture that contained the highest Al content. The Al remained stable in totally tetrahedral coordination after calcination at 550 C. The Al-SBA-15 mesoporous catalyst showed significant catalytic activity for cumene dealkylation, and the activity increased as the amount of zeolite precursor added to the SBA-15 mixture was increased. In preparation for the final phase of the project, the catalyst was embedded into psuedoboemite alumina (catapal B) matrix and then formed into pellets. In the final phase of the project, the pelletized catalyst will be evaluated for the conversion of heavy petroleum feedstocks to naphtha and middle distillates.

  2. IMPROVED CATALYSTS FOR HEAVY OIL UPGRADING BASED ON ZEOLITE Y NANOPARTICLES ENCAPSULATED STABLE NANOPOROUS HOST

    Energy Technology Data Exchange (ETDEWEB)

    Conrad Ingram; Mark Mitchell

    2006-06-20

    Al-SBA-15 mesoporous catalysts with strong Broensted acid sites and Al stabilized in a totally tetrahedral coordination was synthesized from the addition of hydrothermally aged zeolite Y precursor to SBA-15 synthesis mixture under mildly acidic condition of pH 5.5. The materials possessed surface areas between 690 and 850 m{sup 2}/g, pore sizes ranging from 5.6 to 7.5 nm and pore volumes up 1.03 cm{sup 3}, which were comparable to parent SBA-15 synthesized under similar conditions. Up to 2 wt. % Al was present in the most aluminated sample that was investigated, and the Al remained stable in totally tetrahedral coordination, even after calcination at 550 C. The Al-SBA-15 mesoporous catalyst showed significant catalytic activity for cumene dealkylation, and activity increased as the amount of zeolite precursor added to the SBA-15 mixture was increased. The catalyst's activity was not affected by the aging time of the precursor for up to the 24 hr aging time investigated. This method of introducing Al and maintaining it in a total tetrahedral coordination is very effective, in comparison to other direct and post synthesis alumination methods reported. The catalytic performance of the zeolite Y/SBA-15 composite materials will be compared with that of pure SBA-15. The catalysts will then be evaluated for the conversion of heavy petroleum feedstocks.

  3. Liquid and Gaseous Fuel from Waste Plastics by Sequential Pyrolysis and Catalytic Reforming Processes over Indonesian Natural Zeolite Catalysts

    Directory of Open Access Journals (Sweden)

    Mochamad Syamsiro

    2014-08-01

    Full Text Available In this study, the performance of several differently treated natural zeolites in a sequential pyrolysis and catalytic reforming of plastic materials i.e. polypropylene (PP and polystyrene (PS were investigated. The experiments were carried out on two stage reactor using semi-batch system. The samples were degraded at 500°C in the pyrolysis reactor and then reformed at 450°C in the catalytic reformer. The results show that the mordenite-type natural zeolites could be used as efficient catalysts for the conversion of PP and PS into liquid and gaseous fuel. The treatment of natural zeolites in HCl solution showed an increase of the surface area and the Si/Al ratio while nickel impregnation increased the activity of catalyst. As a result, liquid product was reduced while gaseous product was increased. For PP, the fraction of gasoline (C5-C12 increased in the presence of catalysts. Natural zeolite catalysts could also be used to decrease the heavy oil fraction (>C20. The gaseous products were found that propene was dominated in all conditions. For PS, propane and propene were the main components of gases in the presence of nickel impregnated natural zeolite catalyst. Propene was dominated in pyrolysis over natural zeolite catalyst. The high quality of gaseous product can be used as a fuel either for driving gas engines or for dual-fuel diesel engine.

  4. Microporous Zeolites as Catalysts for the Preparation of Decyl Glucoside from Glucose with 1-Decanol by Direct Glucosidation

    Directory of Open Access Journals (Sweden)

    Kyong-Hwan Chung

    2016-12-01

    Full Text Available The catalytic properties of microporous zeolite catalysts were evaluated in the synthesis of decyl glucoside from glucose with 1-decanol by direct glucosidation. The effects of the acidic properties and pore structure of the zeolite catalysts on the glucose conversions and decyl glucoside yields were investigated. The conversions of glucose on the H+ ion-exchanged FAU, MFI, and BEA zeolite catalysts were above 70%. The conversion increased with decreasing acid strength of the catalysts. The highest conversion and yield of decyl glucoside were exhibited on the H-FAU(3 zeolite catalyst. The catalytic activities were enhanced with increasing amounts of acid sites. The selectivity of decyl glucopyranoside increased with decreasing Si/Al values for the same zeolite catalysts. The pore structure of H-FAU zeolite would allow sufficient spatial restriction to produce decyl glucopyranoside through the isomerization of decyl glucofuranoside into decyl glucopyranoside in its extensive pore channels. The selectivities of the decyl glucoside isomers relied significantly on the restricted transition state to the primary products due to their pore topologies.

  5. IMPROVED CATALYSTS FOR HEAVY OIL UPGRADING BASED ON ZEOLITE Y NANOPARTICLES ENCAPSULATED IN STABLE NANOPOROUS HOST

    Energy Technology Data Exchange (ETDEWEB)

    Conrad Ingram; Mark Mitchell

    2005-03-31

    The objectives of this project are to synthesis nanocrystals of highly acidic zeolite Y, encapsulate them within the channels of mesoporous (nanoporous) silicates or nanoporous organosilicates and evaluate the ''zeolite Y/Nanoporous host'' composites as catalysts for the upgrading of heavy petroleum feedstocks. Our results to date are summarized as follows. The synthesis of high surface ordered nanoporous silica of expanded pore diameter of 25 nm (larger than the standard size of 8.4 nm) using trimethylbenzene as a pore size expander was accomplished. The synthesis of zeolite Y nanoparticles with median pore size of approximately 50 nm (smaller than the 80 nm typically obtained with TMAOH) using combined TMABr/TMAOH as organic additives was also accomplished. The successful synthesis of zeoliteY/Nanoporous host composite materials by sequential combination of zeolite precursors and nanoporous material precursor mixtures was implied based on results from various characterization techniques such as X-Ray diffraction, infrared spectra, thermal analysis, porosimetry data. The resulting materials showed pore sizes up to 11 nm, and infrared band at 570 cm{sup -1} suggesting the presence of both phases. New results indicated that good quality highly ordered nanoporous silica host can be synthesized in the presence of zeolite Y seed precursor depending on the amount of precursor added. Preliminary research on the catalytic performance of the materials is underway. Probe acid catalyzed reactions, such as the cracking of cumene is currently being conducted. Work in the immediate future will be focused on the following three areas: (1) Further characterization of all-silica and aluminosilicate mesoporous materials with expanded pore sizes up to 30 nm will continue; (2) Research efforts to reduce the average particle size of zeolite nanoparticles down to 35-30 nm will continue; (3) Further synthesis of ZeoliteY/Nanoporous host composite catalysts of

  6. Suppression of methane formation during Fisher-Tropsch synthesis using manganese-cobalt oxide supported on H-5A zeolite as a catalyst

    Institute of Scientific and Technical Information of China (English)

    Syed Tajammul Hussain; Muhammad Mazhar; Muhammad Arif Nadeem

    2009-01-01

    In Fischer-Tropsch synthesis reaction, methane formation is one of the side reactions which must be suppressed in order to get better catalytic selectivity for light olefins. In the present study, we have modified cobalt based Fischer-Tropsch catalyst and developed a process to minimize methane production, consequently to produce maximum yield of light olefins. Manganese-cobalt oxide supported on H-5A zeolite catalyst was synthesized using modified H-5A zeolite, to increase its surface acid sites. Increased acidity of zeolite plays a major part in the suppression of methane formation during the Fischer-Tropsch reaction. The modified zeolite results in the electronic modification of catalyst surface by creating new active catalytic sites. The results are compared with other supported catalysts along with unmodified zeolite. Appreciable reduction in methane formation is achieved on modified zeolite supported catalyst in comparison with unsupported catalyst.

  7. Catalytic wet peroxide oxidation of azo dye (Congo red) using modified Y zeolite as catalyst.

    Science.gov (United States)

    Kondru, Arun Kumar; Kumar, Pradeep; Chand, Shri

    2009-07-15

    The present study explores the degradation of azo dye (Congo red) by catalytic wet peroxide oxidation using Fe exchanged commercial Y zeolite as a catalyst. The effects of various operating parameters like temperature, initial pH, hydrogen peroxide concentration and catalyst loading on the removal of dye, color and COD from an aqueous solution were studied at atmospheric pressure. The percent removals of dye, color and COD at optimum pH(0) 7, 90 degrees C using 0.6 ml H(2)O(2)/350 ml solution and 1g/l catalyst was 97% (in 4h), 100% (in 45 min) and 58% (in 4h), respectively. The % dye removal has been found to be less in comparison to % color removal at all conditions, e.g. dye removal in 45 min and at above conditions was 82%, whereas the color removal was 100%. The results indicate that the Fe exchanged Y zeolite is a promising catalyst for dye removal. Fe exchanged catalyst is characterized using XRD, SEM/EDAX, surface area analyzer and FTIR. Though the dye, color and COD removals were maximum at pH(0) 2 but as the leaching of Fe from the catalyst was more in acidic pH range, pH(0) 7 was taken as operating pH due to almost comparable removals as of pH(0) 2 and no leaching of Fe ions.

  8. IMPROVED CATALYSTS FOR HEAVY OIL UPGRADING BASED ON ZEOLITE Y NANOPARTICLES ENCAPSULATED STABLE NANOPOROUS HOST

    Energy Technology Data Exchange (ETDEWEB)

    Conrad Ingram; Mark Mitchell

    2005-03-21

    The objectives of this project are to synthesis nanocrystals of highly acidic zeolite Y, encapsulate them within the channels of mesoporous (nanoporous) silicates or nanoporous organosilicates and evaluate the ''zeolite Y/Nanoporous host'' composites as catalysts for the upgrading of heavy petroleum feedstocks. Our results to date are summarized as follows. The synthesis of high surface ordered nanoporous silica of expanded pore diameter of 25 nm (larger than the standard size of 8.4 nm) using trimethylbenzene as a pore size expander was accomplished. The synthesis of zeolite Y nanoparticles with median pore size of approximately 50 nm (smaller than the 80 nm typically obtained with TMAOH) using combined TMABr/TMAOH as organic additives was also accomplished. The successful synthesis of zeoliteY/Nanoporous host composite materials by sequential combination of zeolite precursors and nanoporous material precursor mixtures was implied based on results from various characterization techniques such as X-Ray diffraction, infrared spectra, thermal analysis, porosimetry data. The resulting materials showed pore sizes up to 11 nm, and infrared band at 570 cm{sup -1} suggesting the presence of both phases. Work in the immediate future will be focused on the following three areas: (1) Further characterization of all-silica and aluminosilicate mesoporous materials with expanded pore sizes up to 30 nm will continue; (2) Research efforts to reduce the average particle size of zeolite nanoparticles down to 35-30 nm will continue; (3) Further synthesis of polymer-SBA15 nanocomposites will be conducted by changing the amount and chemistry of the zeolitic precursors added; and (4) Investigation on the catalytic properties of the materials using probe catalytic reactions (such as cumene cracking), followed by catalytic testing for heavy oil conversion.

  9. Metal-Exchanged β Zeolites as Catalysts for the Conversion of Acetone to Hydrocarbons

    Directory of Open Access Journals (Sweden)

    Aurora J. Cruz-Cabeza

    2012-01-01

    Full Text Available Various metal-β zeolites have been synthesized under similar ion-exchange conditions. During the exchange process, the nature and acid strength of the used cations modified the composition and textural properties as well as the Brönsted and Lewis acidity of the final materials. Zeolites exchanged with divalent cations showed a clear decrease of their surface Brönsted acidity and an increase of their Lewis acidity. All materials were active as catalysts for the transformation of acetone into hydrocarbons. Although the protonic zeolite was the most active in the acetone conversion (96.8% conversion, the metal-exchanged zeolites showed varied selectivities towards different products of the reaction. In particular, we found the Cu-β to have a considerable selectivity towards the production of isobutene from acetone (over 31% yield compared to 7.5% of the protonic zeolite. We propose different reactions mechanisms in order to explain the final product distributions.

  10. Improved Catalysts for Heavy Oil Upgrading Based on Zeolite Y Nanoparticles Encapsulated Stable Nanoporous Host

    Energy Technology Data Exchange (ETDEWEB)

    Conrad Ingram; Mark Mitchell

    2007-03-31

    The addition of hydrothermally-aged zeolite Y precursor to an SBA-15 synthesis mixture under a mildly acidic condition resulted in the formation of a mesoporous aluminosilicate catalyst, AlSBA-15. The Al-SBA-15 mesoporous catalyst contains strong Br{umlt o}nsted acid sites and aluminum (Al) stabilized in a totally tetrahedral coordination. The physicochemical characteristics of the catalyst varied as a function of the synthesis conditions. The catalyst possessed surface areas ranging between 690 and 850 m{sup 2}/g, pore sizes ranging from 5.6 to 7.5 nm, and pore volumes up 1.03 cm{sup 3}, which were comparable to the parent SBA-15 synthesized under similar conditions. Two wt % Al was present in the catalyst that was obtained from the reaction mixture that contained the highest Al content. The Al remained stable in totally tetrahedral coordination after calcination at a temperature of 550 C. The Al-SBA-15 mesoporous catalyst showed significant catalytic activity for cumene dealkylation, and the activity increased as the amount of zeolite precursor added to the SBA-15 mixture was increased. In preparation for the final phase of the project, the catalyst was embedded into a psuedoboemite alumina (catapal B) matrix and then formed into pellets. In the final phase of the project, the pelletized catalyst is being evaluated for the conversion of a heavy petroleum feedstock to naphtha and middle distillates. This phase was significantly delayed during the past six months due to a serious malfunction of the fume hoods in the Clark Atlanta University's Research Center for Science and Technology, where the project is being conducted. The fume hood system was repaired and the catalyst evaluation is now underway.

  11. Efficient Isomerization of Glucose to Fructose over Zeolites in Consecutive Reactions in Alcohol and Aqueous Media

    DEFF Research Database (Denmark)

    Shunmugavel, Saravanamurugan; Paniagua, Marta; Melero, Juan A

    2013-01-01

    Isomerization reactions of glucose were catalyzed by different types of commercial zeolites in methanol and water in two reaction steps. The most active catalyst was zeolite Y, which was found to be more active than the zeolites beta, ZSM-5, and mordenite. The novel reaction pathway involves...

  12. Evaluation of photocatalytic activities of supported catalysts on NaX zeolite or activated charcoal

    Energy Technology Data Exchange (ETDEWEB)

    Brites-Nóbrega, Fernanda F. de [Chemical Engineering Department, Universidade Estadual de Maringá (UEM), Av. Colombo, 5790, CEP 87020-900 Maringá, PR (Brazil); Sanitary and Environmental Engineering Department, Universidade Federal de Minas Gerais (UFMG), Av. Antônio Carlos, 6627, Campus Pampulha, Belo Horizonte, MG (Brazil); Polo, Aldino N.B.; Benedetti, Angélica M. [Chemical Engineering Department, Universidade Estadual do Oeste do Paraná (UNIOESTE), Rua da Faculdade, 645, CEP 85903-000 Toledo, PR (Brazil); Leão, Mônica M.D. [Sanitary and Environmental Engineering Department, Universidade Federal de Minas Gerais (UFMG), Av. Antônio Carlos, 6627, Campus Pampulha, Belo Horizonte, MG (Brazil); Slusarski-Santana, Veronice, E-mail: veronice.santana@unioeste.br [Chemical Engineering Department, Universidade Estadual do Oeste do Paraná (UNIOESTE), Rua da Faculdade, 645, CEP 85903-000 Toledo, PR (Brazil); Fernandes-Machado, Nádia R.C. [Chemical Engineering Department, Universidade Estadual de Maringá (UEM), Av. Colombo, 5790, CEP 87020-900 Maringá, PR (Brazil)

    2013-12-15

    Highlights: • The synergic effect between ZnO and NaX was positive, which increased its activity. • The best results were obtained at pH 3 and 9 with ZnO/NaX and at pH 3 with Nb{sub 2}O{sub 5}/AC. • High degradation and considerable mineralization were attained with 10% ZnO/NaX. • ZnO and Nb{sub 2}O{sub 5} supported on NaX and AC are promising alternatives as photocatalysts. -- Abstract: This study aimed to evaluate the photocatalytic activity of ZnO and Nb{sub 2}O{sub 5} catalysts, both supported on NaX zeolite and activated charcoal (AC). The synergistic effect between oxide and support and the influence of solution pH (3, 7 and 9) on photocatalytic degradation of reactive blue 5G (C.I. 222) were analyzed. The catalysts Nb{sub 2}O{sub 5}/NaX, Nb{sub 2}O{sub 5}/AC and ZnO/NaX, ZnO/AC with 5 and 10% (wt%) were prepared by wet impregnation. The results showed that the catalysts exhibit quite different structural and textural properties. The synergic effect between ZnO and NaX support was higher than that with the activated charcoal, showing that these catalysts were more efficient. The most photoactive catalyst was 10% ZnO/NaX which showed 100% discoloration of the dye solution at pH 3, 7 and 9 after 0.5, 5 and 2 h of irradiation, respectively. The hydrolytic nature of zeolite favored the formation of surface hydroxyl radicals, which increased the activity of the photocatalyst. Thus, catalysts supported on NaX zeolite are promising for use in photocatalysis.

  13. Electrophilic Aromatic Iodine Substitution of 1-[(p-TolyliminoMethyl]-Naphthalen-2-Ol In Zeolite Catalyst

    Directory of Open Access Journals (Sweden)

    Murat Gündüz

    2011-12-01

    Full Text Available In this study, the naphtholic Schiff base has been reacted with iodine in the catalyst of natural zeolite clinoptilolite in order to synthesize iodine substituted Schiff base. The isolated product structure has been determined by IR, UV, 1H-NMR, 13C-NMR, Mass spectroscopy and elemental analysis. Under our reaction conditions it's found that the iodine is substituted to the phenyl ring of the naphtholic Schiff base.

  14. Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts

    Science.gov (United States)

    Devaraj, Arun; Vijayakumar, Murugesan; Bao, Jie; Guo, Mond F.; Derewinski, Miroslaw A.; Xu, Zhijie; Gray, Michel J.; Prodinger, Sebastian; Ramasamy, Karthikeyan K.

    2016-11-01

    The formation of carbonaceous deposits (coke) in zeolite pores during catalysis leads to temporary deactivation of catalyst, necessitating regeneration steps, affecting throughput, and resulting in partial permanent loss of catalytic efficiency. Yet, even to date, the coke molecule distribution is quite challenging to study with high spatial resolution from surface to bulk of the catalyst particles at a single particle level. To address this challenge we investigated the coke molecules in HZSM-5 catalyst after ethanol conversion treatment by a combination of C K-edge X-ray absorption spectroscopy (XAS), 13C Cross polarization-magic angle spinning nuclear magnetic resonance (CP-MAS NMR) spectroscopy, and atom probe tomography (APT). XAS and NMR highlighted the aromatic character of coke molecules. APT permitted the imaging of the spatial distribution of hydrocarbon molecules located within the pores of spent HZSM-5 catalyst from surface to bulk at a single particle level. 27Al NMR results and APT results indicated association of coke molecules with Al enriched regions within the spent HZSM-5 catalyst particles. The experimental results were additionally validated by a level-set–based APT field evaporation model. These results provide a new approach to investigate catalytic deactivation due to hydrocarbon coking or poisoning of zeolites at an unprecedented spatial resolution.

  15. Zeolite Based SCR Catalysts - An Interesting Alternative To Vanadia-Titania Systems

    Energy Technology Data Exchange (ETDEWEB)

    Devadas, M.; Kroecher, O.; Wokaun, A.

    2004-03-01

    Metal exchanged zeolite catalysts were tested for the selective catalytic reduction of NO{sub x} with ammonia (NH{sub 3}-SCR) and compared with a vanadia based catalyst. With pure NO in the feed Cu-ZSM5 exhibited a better NO{sub x} conversion than Fe-ZSM5 and V{sub 2}O{sub 5}/WO{sub 3}-TiO{sub 2} at all temperatures. The main drawback of Cu-ZSM5 is the required excess of ammonia due to oxidation of NH{sub 3} to N{sub 2} (SCO). For a feed ratio of NO:NO{sub 2} = 0.5, all catalysts showed a high activity at elevated temperatures, but Fe-ZSM5 and Cu-ZSM5 performed better than the vanadia catalyst at lower temperatures. (author)

  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. 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.

  18. Green chemistry perspectives of methane conversion via oxidative methylation of aromatics over zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Adebajo, M.O. [University of Queensland, St Lucia, Qld. (Australia)

    2007-06-15

    This paper provides a general overview of the recent work that we and other researchers have done on the utilisation of methane for catalytic methylation of aromatic compounds and for direct coal liquefaction for the production of liquid hydrocarbons. In particular, the paper presents a detailed description of more recent substantial experimental evidence that we have provided for the requirement of oxygen as a stoichiometry reactant for benzene methylation with methane over moderately acidic zeolite catalysts. The reaction, which has been termed 'oxidative methylation', was thus postulated to involve a two-step mechanism involving intermediate methanol formation by methane partial oxidation, followed by benzene methylation with methanol in the second step. However, strongly acidic zeolites can cause cracking of benzene to yield methylated products in the absence of oxygen. The participation of methane and oxygen, and the effective use of zeolite catalysts in this methylation reaction definitely have some positive green chemistry implications. Thus, the results of these previous studies are also discussed in this review in light of the principles and tools of green chemistry. Various metrics were used to evaluate the greenness, cost-effectiveness, and material and energy efficiency of the oxidative methylation reaction.

  19. Session 6: Highly active Pt/zeolite catalysts for combustion of C{sub 2}-C{sub 4} alkanes

    Energy Technology Data Exchange (ETDEWEB)

    Garetto, T.F.; Rincon, E.; Apesteguia, C.R. [Instituto de Investigaciones en Catalisis y Petroquimica -INCAPE- (UNL-CONICET), Santa Fe (Argentina)

    2004-07-01

    In an attempt for developing more active Pt-based catalysts for lower-alkane combustion, we investigate in this work the deep oxidation of C{sub 2}-C{sub 4} alkanes over Pt-based catalysts. Results show that the lower alkane oxidation turnover rates are more than two orders of magnitude higher on Pt/zeolites compared to Pt/Al{sub 2}O{sub 3} catalyst. (authors)

  20. Theoretical study of the interaction between vanadium oxide and HY-Zeolite elucidating loss activity of the catalyst

    Directory of Open Access Journals (Sweden)

    Irineo Pedro Zaragoza

    2017-01-01

    Full Text Available The study of the interaction between vanadium oxide and the HY-zeolite using molecular dynamics interaction was carried out for two systems: i when vanadium oxide penetrates a zeolite ring at its center, and ii when vanadium oxide impacts the zeolite surface model. The dynamical effects are used to investigate the reduced activity and eventual degradation of the catalyst for the vanadium oxide presence. In the first case, we observe the breaking of an OH-bond that belongs to the acid site. This is related to an initial loss activity stage of the catalyst. In the second case, vanadium oxide is weakly adsorbed onto the zeolite surface velocity depending. Density functional theory, with nonlocal exchange and correlation functional and the basis set of double numerical accuracy, is used to analyze the electronic structure. It was used in combination with Born-Oppenheimer dynamics to perform calculations.

  1. Zeolites Modified Metal Cations as Catalysts in Hydrocarbon Oxidation and the Alkyl Alcohol

    Directory of Open Access Journals (Sweden)

    Agadadsh Makhmud Aliyev

    2014-09-01

    Full Text Available The results of studies on the creation of highly metalltceolitnyh systems and the study of their catalytic activities in the oxidation of lower olefin hydrocarbons (ethylene to acetaldehyde, acetone, propylene, butylene methyl ethyl ketone; aliphatic C1-C5 alcohols to their corresponding aldehydes, ketones, carboxylic acids and carboxylic acid esters; oxidative dehydrogenation of naphthenes in the alicyclic diene hydrocarbons and the oxidative dimerization of methane to acetylene. It has been established that the selectivity of these catalysts determined optimal combination of metal components with the acidity and the structure of the zeolite. Selected highly effective catalysts for the reactions studied. Based on the results of experimental studies of the kinetics of the reactions of oxidation of lower olefin hydrocarbons and aliphatic alcohols, the oxidative dehydrogenation of naphthenes and oxidative coupling of methane on the synthesized catalysts are represented by their probable stepwise mechanism and kinetic models developed reactions.

  2. Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Devaraj, Arun; Vijayakumar, Murugesan; Bao, Jie; Guo, Mond F.; Derewinski, Miroslaw A.; Xu, Zhijie; Gray, Michel J.; Prodinger, Sebastian; Ramasamy, Karthikeyan K.

    2016-11-23

    The nanoscale compositional mapping of fresh HZSM-5 catalyst synthesized using hydrothermal process as well as after just steaming and after ethanol conversion reaction for 72 hours at realistic catalytic conditions was investigated using atom probe tomography. Atom probe tomography permitted direct atomic scale imaging of non-uniform distribution of Al within the HZSM-5 as well as for the first time image the hydrocarbon coking after ethanol reaction. Clear evidences for existence of multiple C-H molecular species which appear to aggregate as clusters within the pores of spent HZSM-5 catalyst materials is provided. These results provide evidence for the ability of atom probe tomography, a powerful 3D characterization tool in interrogating the atomic scale chemistry of zeolite catalyst materials at industrially relevant catalytic conditions.

  3. Hydrogenation of carbon monoxide over the mixed catalysts composed of cobalt-nickel/manganese oxide-zirconium oxide and zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ishihara, Tatsumi; Iwakuni, Hideharu; Eguchi, Koichi; Arai, Hiromichi (Kyushu Univ., Fukuoka (Japan))

    1991-08-15

    Mechanical mixtures of Co-Ni/MnO-ZrO2 and zeolite were used as catalysts for the selective synthesis of gasoline by carbon monoxide hydrogenation. Formation of branched alkanes was promoted, but that of hydrocarbons higher than a carbon number of 10 was suppressed by a combination with zeolite. The reactivity of zeolite for higher hydrocarbons has the decisive role in the product distribution as result of using these mixed catalysts, and thus the product distribution strongly depends on the type of zeolite. Since the hydrogenolysis of higher hydrocarbons proceeds on the strong acid sites, the formation of branched alkanes was promoted by increasing the aluminium content in the zeolite. Ammonia temperature-programmed desorption suggests that increasing the aluminium content in the zeolite increases the number of strong acid sites, but weakens the average strength of the acid sites. Pentasil zeolite with an aluminium content of 1.32 mmolg{sup -1} is effective for enhancing the yield of gasoline as well as its octane number. 8 figs., 1 tab., 20 refs.

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

    Directory of Open Access Journals (Sweden)

    K. Maduna Valkaj

    2015-01-01

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

  5. Selective Production of Aromatics from 2-Octanol on Zinc Ion-Exchanged MFI Zeolite Catalysts

    Directory of Open Access Journals (Sweden)

    Masakazu Iwamoto

    2015-12-01

    Full Text Available The aromatization of 2-octanol derived from castor oil as a byproduct in the formation of sebacic acid was investigated on various zeolite catalysts. Zn ion-exchanged MFI (ZSM-5 zeolites with small silica/alumina ratios and zinc contents of 0.5 to 2.0 wt. % were determined to exhibit good and stable activity for the reaction at 623 to 823 K. The yield of aromatics was 62% at 773 K and the space velocity 350 to 1400 h−1. The temperature and contact time dependences of the product distributions indicated the reaction pathways of 2-octanol→dehydration to 2-octene→decomposition to C5 and C3 compounds→further decomposition to small alkanes and alkenes→aromatization with dehydrogenation. Alcohols with carbon numbers of 5 to 8 exhibited similar distributions of products compared to 2-octanol, while corresponding carbonyl compounds demonstrated different reactivity.

  6. Selective preparation of zeolite X and A from flyash and its use as catalyst for biodiesel production.

    Science.gov (United States)

    Volli, Vikranth; Purkait, M K

    2015-10-30

    This work discusses the utilization of flyash for synthesis of heterogeneous catalyst for transesterification. Different types of zeolites were synthesized from alkali fusion followed by hydrothermal treatment of coal flyash as source material. The synthesis conditions were optimized to obtain highly crystalline zeolite based on degree of crystallinity and cation exchange capacity (CEC). The effect of CEC, acid treatment, Si/Al ratio and calcination temperature (800, 900 and 1000 °C) on zeolite formation was also studied. Pure, single phase and highly crystalline zeolite was obtained at flyash/NaOH ratio (1:1.2), fusion temperature (550 °C), fusion time (1 h), hydrothermal temperature (110 °C) and hydrothermal time (12h). The synthesized zeolite was ion-exchanged with potassium and was used as catalyst for transesterification of mustard oil to obtain a maximum conversion of 84.6% with 5 wt% catalyst concentration, 12:1 methanol to oil molar ratio, reaction time of 7 h at 65 °C. The catalyst was reused for 3 times with marginal reduction in activity.

  7. Zeolites

    Science.gov (United States)

    1992-01-01

    Zeolites are crystalline aluminosilicates that have complex framework structures. However, there are several features of zeolite crystals that make unequivocal structure determinations difficult. The acquisition of reliable structural information on zeolites is greatly facilitated by the availability of high-quality specimens. For structure determinations by conventional diffraction techniques, large single-crystal specimens are essential. Alternatively, structural determinations by powder profile refinement methods relax the constraints on crystal size, but still require materials with a high degree of crystalline perfection. Studies conducted at CAMMP (Center for Advanced Microgravity Materials Processing) have demonstrated that microgravity processing can produce larger crystal sizes and fewer structural defects relative to terrestrial crystal growth. Principal Investigator: Dr. Albert Sacco

  8. Hierarchical zeolites: progress on synthesis and characterization of mesoporous zeolite single crystal catalysts

    DEFF Research Database (Denmark)

    Kustova, Marina; Egeblad, Kresten; Christensen, Claus H.

    2007-01-01

    in a hierarchical pore size distribution. In this work, the preparation of mesoporous ZSM-12 single crystal catalysts using a new improved procedure for directly introducing carbon in the reaction mixture is reported. The microwave heating technique is also applied for the synthesis of mesoporous silicalite-1...... single crystals using this direct introduction of carbon into the reaction mixture. All samples were characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), temperature-programmed desorption of ammonia (NH3-TPD), and N-2 adsorption...

  9. Elaboration of new method of enzyme adsorption on silicalite and nano beta zeolite for amperometric biosensor creation

    Directory of Open Access Journals (Sweden)

    Soldatkin O. O.

    2014-07-01

    Full Text Available Aim. Optimization of a new method of enzyme immobilization for amperometric biosensor creation. Methods. The amperometric biosensor with glucose oxidase immobilized on zeolites as bioselective elements and platinum disk electrode as transducers of biochemical signal into the electric one was used in the work. Results. The biosensors based on glucose oxidase adsorbed on zeolites were characterized by a higher sensitivity to glucose and a better inter-reproducibility. The best analytical characteristics were obtained for the biosensors based on nano beta zeolite. It has been found that an increase in the amount of zeolite on the surface of amperometric transducer may change such biosensor parameters as sensitivity to the substrate and duration of the analysis. Conclusions. The proposed method of enzyme immobilization by adsorption on zeolites is shown to be quite promising in the development of amperometric biosensors and therefore should be further investigated.

  10. Pure Silica Zeolite Beta Membrane: A Potential Low Dielectric Constant Material For Microprocessor Application

    Science.gov (United States)

    Fong, Yeong Yin; Bhatia, Subhash

    The semiconductor industry needs low dielectric constant (low k-value) materials for more advance microprocessor and chips by reducing the size of the device features. In fabricating these contents, a new material with lower k-value than conventional silica (k = 3.9-4.2) is needed in order to improve the circuit performance. The choice of the inorganic zeolite membrane is an attractive option for low k material and suitable for microprocessor applications. A pure silica zeolite beta membrane was synthesized and coated on non-porous stainless steel support using insitu crystallization in the presence of tetraethylammonium hydroxide, TEA (OH), as structure directing agent, fumed silica, HF and deionized water at pH value of 9. The crystallization was carried out for the duration of 14 days under hydrothermal conditions at 130°C. The membrane was characterized by thermogravimetric analysis (TGA), nitrogen adsorption and Scanning Electron Microscope (SEM). SEM results show a highly crystalline; with a truncated square bipyramidal morphology of pure silica zeolite beta membrane strongly adhered on the non-porous stainless steel support. In the present work, the k-value of the membrane was measured as 2.64 which make it suitable for the microprocessor applications.

  11. Hydrothermal Aging Effects on Fe/SSZ-13 and Fe/Beta NH3–SCR Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Gao, Feng; Szanyi, János; Wang, Yilin; Schwenzer, Birgit; Kollár, Márton; Peden, Charles H. F.

    2016-05-05

    Cu/SSZ-13 has been successfully commercialized as a diesel engine exhaust aftertreatment SCR catalyst in the past few years. This catalyst, however, displays undesirable NH3-SCR selectivity at elevated reaction temperature (≥ 350 C) after hydrothermal aging. Fe/zeolites, despite the fact that most of them degrade beyond tolerance after hydrothermal aging at temperatures ≥ 650 C, typically maintain good SCR selectivities. In recent years, Fe/beta has been identified as one of the more robust Fe/zeolites for use in NH3-SCR, where activity maintains even after hydrothermal aging at 750 C. Very recently, we, for the first time, synthesized and tested NH3-SCR performance for fresh and hydrothermally aged Fe/SSZ-13 catalysts. This study demonstrated that Fe/SSZ-13 is also a promising robust SCR catalyst, especially for high-temperature applications. In the present study, we compare catalytic performance between Fe/SSZ-13 and Fe/beta with similar Fe loadings and Si/Al ratios. Special attention is paid to effects from hydrothermal aging, aiming to understanding similarities and differences between these two catalysts. The authors gratefully acknowledge the US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Vehicle Technologies Program for the support of this work. The research described in this paper was performed at the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the US DOE by Battelle.

  12. Correlating metal poisoning with zeolite deactivation in an individual catalyst particle by chemical and phase sensitive X-ray microscopy

    NARCIS (Netherlands)

    Ruiz-Martinez, J.; Beale, A.M.; Deka, U.; O'Brien, M.G.; Quinn, P.D.; Mosselmans, J.F.W.; Weckhuysen, B.M.

    2013-01-01

    Fluid catalytic cracking (FCC) is the main conversion process used in oil refineries. An X-ray microscopy method is used to show that metal poisoning and related structural changes in the zeolite active material lead to a non-uniform core–shell deactivation of FCC catalyst particles. The study links

  13. Spatial Distribution of Zeolite ZSM-5 within Catalyst Bodies Affects Selectivity and Stability of Methanol-to-Hydrocarbons Conversion

    NARCIS (Netherlands)

    Castaño, P.; Ruiz-Martinez, J.; Epelde, E.; Gayubo, A.G.; Weckhuysen, B.M.

    2013-01-01

    Solid acids, such as zeolites, are used as catalyst materials in a wide variety of important crude oil refinery, bulk chemical synthesis, and green processes. Examples include fluid catalytic cracking (FCC),[1] methanol-to-hydrocarbons (MTH) conversion,[ 2] plastic waste valorization,[3] and biomass

  14. IMPROVED CATALYSTS FOR HEAVY OIL UPGRADING BASED ON ZEOLITE Y NANOPARTICLES ENCAPSULATED IN STABLE NANOPOROUS HOST

    Energy Technology Data Exchange (ETDEWEB)

    Conrad Ingram; Mark Mitchell

    2005-11-15

    Composite materials of SBA-15/zeolite Y were synthesized from zeolite Y precursor and a synthesis mixture of mesoporous silicate SBA-15 via a hydrothermal process in the presence of a slightly acidic media of pH 4-6 with 2M H{sub 2}SO{sub 4}. The SBA-15/ZY composites showed Type IV adsorption isotherms, narrow BJH average pore size distribution of 4.9 nm, surface areas up to 800 m{sup 2}2/g and pore volumes 1.03 cm{sup 3}, all comparable to pure SBA-15 synthesized under similar conditions. Chemical analysis revealed Si/Al ratio down to 8.5 in the most aluminated sample, and {sup 27}AlSS MAS NMR confirmed aluminum was in tetrahedral coordination. This method of introduction of Al in pure T{sub d} coordination is effective in comparison to other direct and post synthesis alumination methods. Bronsted acid sites were evident from a pyridinium peak at 1544 cm-1 in the FTIR spectrum after pyridine adsorption, and from NH{sub 3} -TPD experiments. SBA-15/ZY composites showed significant catalytic activities for the dealkylation of isopropylbenzene to benzene and propene, similar to those of commercial zeolite Y. It was observed that higher conversion for catalysts synthesized with high amount of ZY precursor mixture added to the SBA-15. Over all the composites has shown good catalytic activity. Further studies will be focused on gaining a better understand the nature of the precursor, and to characterize and to locate the acid sites in the composite material. The composite will also be evaluated for heavy oil conversion to naphtha and middle distillates.

  15. Synthesis of zeolite beta with pretreated rice husk silica and its transformation to ZSM-12

    Energy Technology Data Exchange (ETDEWEB)

    Loiha, Sirinuch [Material Chemistry Research Unit, School of Chemistry, Institute of Science, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); Synchrotron Light Research Institute (Public Organization), Nakhon Ratchasima 30000 (Thailand); Prayoonpokarach, Sanchai [Material Chemistry Research Unit, School of Chemistry, Institute of Science, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); Songsiriritthigun, Prayoon [Synchrotron Light Research Institute (Public Organization), Nakhon Ratchasima 30000 (Thailand); Wittayakun, Jatuporn, E-mail: jatuporn@sut.ac.th [Material Chemistry Research Unit, School of Chemistry, Institute of Science, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); Center of Environmental and Hazardous Waste Management (EHWM), Thammasat University, Pathumtani 12120 (Thailand)

    2009-06-15

    Silica with 98% purity was prepared from rice husk by acid leaching and used as a silica source for the syntheses of zeolite beta (Beta) under hydrothermal conditions with gel Si/Al ratios of 8, 13, 15, 20, 50, 100, 150, and 200. Based on powder X-ray diffraction patterns, samples with gel Si/Al ratios of 8-20 contained only the pure phase of Beta and the highest relative crystallinity was observed in the Beta with gel Si/Al ratio of 13. This sample was further characterized by scanning electron microscopy, particle size analyzer and N{sub 2} adsorption analysis. The Beta particles were sphere shaped with the average particle size of 1.5 {mu}m and a surface area of 670 m{sup 2} g{sup -1}. The samples with gel Si/Al ratios ranging from 50 to 200 showed mixed phases of Beta and ZSM-12, and the latter phase was more dominant as the Si/Al ratio increased.

  16. A Zeolite Imidazolate Framework ZIF-8 Catalyst for Friedel-Crafts Acylation

    Institute of Scientific and Technical Information of China (English)

    LienT.L.NGUYEN; Ky K.A.LE; Nam T.S.PHAN

    2012-01-01

    A zeolite imidazolate framework,ZIF-8,was synthesized and characterized by dynamic laser light scattering,X-ray powder diffraction,scanning electron microscopy,transmission electron microscopy,thermogravimetric analysis,Fourier transform infrared,atomic absorption spectrophotometry,and nitrogen adsorption measurements.The ZIF-8 was highly crystalline and porous with a surface area of over 1600 m2/g.Friedel-Crafts acylation of anisole and benzoyl chloride proceeded well in the presence of ZIF-8 (2-6 mol%) without the need for an inert atmosphere.The reaction afforded a selectivity of 93%-95% to the p-isomer.The solid catalyst can be separated from the reaction mixture by simple centrifugation and reused without significant degradation in catalytic activity.There was no leaching of active acid species into the reaction solution.

  17. One-pot hydrothermal synthesis of CuBi co-doped mesoporous zeolite Beta for the removal of NOx by selective catalytic reduction with ammonia

    Science.gov (United States)

    Xie, Zhiguo; Zhou, Xiaoxia; Wu, Huixia; Chen, Lisong; Zhao, Han; Liu, Yan; Pan, Linyu; Chen, Hangrong

    2016-07-01

    A series of CuBi co-doped mesoporous zeolite Beta (CuxBiy-mBeta) were prepared by a facile one-pot hydrothermal treatment approach and were characterized by XRD, N2 adsorption-desorption, TEM/SEM, XPS, H2-TPR, NH3-TPD and in situ DRIFTS. The catalysts CuxBiy-mBeta were applied to the removal of NOx by selective catalytic reduction with ammonia (NH3-SCR), especially the optimized Cu1Bi1-mBeta achieved the high efficiency for the removal of NOx and N2 selectivity, superior water and sulfur resistance as well as good durability. The excellent catalytic performance could be attributed to the acid sites of the support and the synergistic effect between copper and bismuth species. Moreover, in situ DRIFTS results showed that amides NH2 and NH4+ generated from NH3 adsorption could be responsible for the high selective catalytic reduction of NOx to N2. In addition, a possible catalytic reaction mechanism on Cu1Bi1-mBeta for the removal of NOx by NH3-SCR was proposed for explaining this catalytic process.

  18. Effects of Dealumination and Desilication of Beta Zeolite on Catalytic Performance in n-Hexane Cracking

    Directory of Open Access Journals (Sweden)

    Yong Wang

    2016-01-01

    Full Text Available Catalytic cracking of n-hexane to selectively produce propylene on Beta zeolite was carried out. The H-Beta (HB (Si/Al = 77 zeolite showed higher catalytic stability and propylene selectivity than the Al-rich HB (Si/Al = 12, due to its smaller number of acid sites, especially Lewis acid sites (LAS. However, catalytic stability and propylene selectivity in high n-hexane conversions were still not satisfactory. After dealumination with HNO3 treatment, catalytic stability was improved and propylene selectivity during high n-hexane conversions was increased. On the other hand, catalytic stability was not improved after desilication with NaOH treatment, although mesopores were formed. This may be related to the partially destroyed structure. However, propylene selectivity in high n-hexane conversions was increased after alkali treatment. We successfully found that the catalytic stability was improved and the propylene selectivity in high n-hexane conversions was further increased after the NaOH treatment followed by HNO3 treatment. This is due to the decrease in the number of acid sites and the increase in mesopores which are beneficial to the diffusion of coke precursor.

  19. Effect of Reaction Temperature on Biodiesel Production from Chlorella vulgaris using CuO/Zeolite as Heterogeneous Catalyst

    Science.gov (United States)

    Dianursanti; Delaamira, M.; Bismo, S.; Muharam, Y.

    2017-02-01

    Human needs for fossil energy increase every year. Biodiesel is the main way to resolve this world problem. Biodiesel produces from vegetable oil. But then, the alternative way came from the uses of microalgae in Chlorella vulgaris type causes by its simplicity of growing. In the other hand, this microalgae known for its high lipid content by considering several parameter such as light intensity, medium nutrition, pH and also salinity. Lipid content will be extracted by using Bligh-Dryer method which will be reacted with methanol along transesterification. Beside, there come another matter which is the utilization of homogeny catalyst. The difficulty of separation is the main matter so then biodiesel need to be washed in case normalizing the pH and this process will decrease the quality of biodiesel. To resolve this problem, we’ll be using a heterogeneous catalyst, zeolite, with ability to catalyst the process. Zeolite is easier to separate from the biodiesel so there will not be needed washing process. Heterogeneous catalyst work as well as homogeneous. Variation implemented on transesterification included reaction temperature of 40°C, 60°C, and 80°C. Reaction time, catalyst percentage and the solvent amount remain steady on 4 hours, 3% and 1:400. Complete best result obtained at 60°C with the yield of 36,78%. Through this, heterogeneous catalyst CuO/Zeolite proved to have a capability for replacing homogeneous catalyst and simplify the production of biodiesel particularly in separation step.

  20. 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.

  1. Hydrogenation of carbon monoxide over mixed catalysts. Co-Ni/MnO-ZrO sub 2 to zeolite kara naru kongo shokubai wo mochiita issankatanso no suisoka

    Energy Technology Data Exchange (ETDEWEB)

    Ishihara, T.; Iwakuni, H.; Eguchi, K.; Arai, H. (Graduate School of Engineering Sciences, Kyushu Univ., Fukuoka (Japan). Department of Materials Science and Technology)

    1990-07-10

    The mechanical mixtures of Co-Ni/MnO-ZrO {sub 2} and zeolite were used as catalysts for the selective synthesis of gasoline by CO hydrogenation. Formation of branched-paraffins was promoted but that of higher hydrocarbons than carbon number of 10 was suppressed by combination with zeolite. The product distribution strongly depended on the type of zeolite catalyst. Pentasil zeolite was active for the formation of branched-paraffins, probably because of the cracking reaction occurring on the strong acid sites. The formation of branched paraffin was further promoted by ion-exchange with Pt. The mixture of Co-Ni/MnO-ZrO {sub 2} and PtH-pentasil zeolite was very active for the formation of gasoline with high octane number. 34 refs., 10 figs., 2 tabs.

  2. Fenton chemistry-based detemplation of an industrially relevant microcrystalline beta zeolite. Optimization and scaling-up studies

    NARCIS (Netherlands)

    Ortiz-Iniesta, Maria Jesus; Melian-Cabrera, Ignacio

    2015-01-01

    A mild template removal of microcrystalline beta zeolite, based on Fenton chemistry, was optimized. Fenton detemplation was studied in terms of applicability conditions window, reaction rate and scale up. TGA and CHN elemental analysis were used to evaluate the detemplation effectiveness, while 'CP,

  3. Acid Activation of Natural Zeolite with High Content of Iron Oxides in Creation of Selective Sorbents and Catalysts

    Directory of Open Access Journals (Sweden)

    Kadirbekov Kairat

    2017-01-01

    Full Text Available The paper studies the influence of the nature of modifying acids (mineral, organic and heteropolyacids, and their combination on the composition and structure of the iron oxide rich clinoptilolit from Shankanay field in Kazakhstan for creation of selective catalysts in hydracarbon processing and sorbents for extracting ions of lanthanide and actinide elements. It is shown that sequential processing of natural zeolite in optimal conditions, by hydrochloric and sulfosalicylic acids lead to intensive decationization and dealumination, as well as maximum removal of iron ions from the zeolite framework without destroying it. It is found that the combination of activated clinoptilolite with hydrochloric acid and phosphotungstic heteropolyacid contributes to obtain catalyst system with high surface area and acidity.

  4. Influence of n Si/ n Al ratio of HY zeolite catalysts on alkylation of toluene with tert-butanol

    Science.gov (United States)

    Wang, Yuanyuan; Song, Hua; Sun, Xinglong; Song, HuaLin

    2016-12-01

    The highly selective synthesis of 4- tert-butyltoluene from toluene and tert-butanol over HY zeolites was performed in liquid phase. The effect of Si/Al ratio (6.3, 7.5, 11, 12) of HY zeolites on the alkylation performance was studied. The catalysts were characterized by SEM, XRD, FT-IR, and NH3-TPD methods. With increase of Si/Al ratio, the conversion of toluene and the selectivity towards 4- tert-butyltoluene increased gradually. HY-12 was found to be more suitable for the tert-butylation of toluene. When the alkylation reaction was conducted at 180°C for 4 h using HY-12 catalyst, the conversion and the selectivity of 4- tertbutyltoluene reached 40.74 and 70.91%, respectively.

  5. SYNTHESIS OF ZEOLITE SOCONY MOBIL FROM BLUE SILICA GEL AND RICE HUSK ASH AS CATALYSTS FOR HYDROTHERMAL LIQUEFACTION

    OpenAIRE

    SUYITNO; SANURYA PUTRI PURBANINGRUM; DOMINICUS DANARDONO; ALFAITORY EMHEMED SALEM; FATHI A. MANSUR

    2015-01-01

    Renewable biofuels produced by the hydrothermal liquefaction of rice husks have received much attention because of rapid increases in fuel consumption and corresponding declines in fossil fuel resources. To increase biofuel yields, template-free syntheses of Zeolite Socony Mobil (ZSM) catalysts based on blue silica gel and rice husk ash as silica sources were studied. After ZSM synthesis in a closed reactor at 170°C, the crystallinity and crystalline diameters of the products were determined ...

  6. Heteropoly acid encapsulated into zeolite imidazolate framework (ZIF-67) cage as an efficient heterogeneous catalyst for Friedel–Crafts acylation

    Energy Technology Data Exchange (ETDEWEB)

    Ammar, Muhammad; Jiang, Sai; Ji, Shengfu, E-mail: jisf@mail.buct.edu.cn

    2016-01-15

    A new strategy has been developed for the encapsulation of the phosphotungstic heteropoly acid (H{sub 3}PW{sub 12}O{sub 40} denoted as PTA) into zeolite imidazolate framework (ZIF-67) cage and the PTA@ZIF-67(ec) catalysts with different PTA content were prepared. The structure of the catalysts was characterized by XRD, BET, SEM, FT-IR, ICP-AES and TG. The catalytic activity and recovery properties of the catalysts for the Friedel-Crafts acylation of anisole with benzoyl chloride were evaluated. The results showed that 14.6–31.7 wt% PTA were encapsulated in the ZIF-67 cage. The PTA@ZIF-67(ec) catalysts had good catalytic activity for Friedel-Crafts acylation. The conversion of anisole can reach ~100% and the selectivity of the production can reach ~94% over 26.5 wt% PTA@ZIF-67(ec) catalyst under the reaction condition of 120 °C and 6 h. After reaction, the catalyst can be easily separated from the reaction mixture by the centrifugation. The recovered catalyst can be reused five times and the selectivity can be kept over 90%. - Graphical abstract: The PTA@ZIF-67 catalysts with different PTA content were prepared by encapsulating the PTA into ZIF-67 cage and the as-synthesized catalysts exhibited good catalytic activity for the Friedel–Craft acylation of anisole with benzoyl chloride.

  7. Kinetics and Mechanism of Deoxygenation Reactions over Proton-Form and Molybdenum-Modified Zeolite Catalysts

    Science.gov (United States)

    Bedard, Jeremy William

    950 K and atmospheric pressure in an effort to couple deoxygenation and dehydrogenation reaction sequences results instead in a two-zone, stratified bed reactor configuration consisting of upstream oxygenate/CH4 reforming and downstream CH4 dehydroaromatization. X-ray absorption spectroscopy and chemical transient experiments show that molybdenum carbide is formed inside zeolite micropores during CH4 reactions. The addition of an oxygenate co-feed causes oxidation of the active molybdenum carbide catalyst while producing CO and H2 until completely converted. Forward rates of C6H6 synthesis are unperturbed by the introduction of an oxygenate co-feed after rigorously accounting for the thermodynamic reversibility caused by the H2 produced in oxygenate reforming reactions and the fraction of the active catalyst deemed unavailable for CH 4 dehydroaromatization. All effects of co-processing C1-2 oxygenates and molecular H2 with CH4 can be interpreted in terms of an approach to equilibrium. Co-processing H2O, CO2, or light (C1-2, C/Heff biomass sources. This research addresses these challenges at fundamental and applied levels as it offers the potential to convert readily available biomass to commodity chemicals and fuels while simultaneously examining the elementary concepts of deoxygenation reactions on catalytic surfaces.

  8. NiMo/Al2O3 catalyst containing nano-sized zeolite Y for deep hydrodesulfurization and hydrodenitrogenation of diesel

    Institute of Scientific and Technical Information of China (English)

    Hailiang Yin; Tongna Zhou; Yunqi Liu; Yongming Chai; Chenguang Liu

    2011-01-01

    Two mixed-matrix NiMo/Al2O3 catalysts containing nano- and micro-sized zeolite Y have been prepared to explore the size effect of zeolite Y particle on the hydrodesulfurization (HDS) and hydrodenitrogenation (HDN) activities of fluid catalytic cracking (FCC) diesel.They were characterized by SEM,BET,XRD,H2-TPR,NH3-TPD and HRTEM.The results show that the catalyst containing nano-sized zeolite Y possesses larger average pore diameter,higher pore volume,weaker and lesser acid sites,more easily reducible metal phases,shorter MoS2 slabs and more slab layers than the catalyst containing micro-sized zeolite Y.The catalysts were also evaluated with a high-pressure fixed-bed reactor using real FCC diesel as feed.The results display that the catalyst containing nano-sized zeolite Y bears higher HDS and HDN activities and exhibits higher relative rate constant for the removal of total sulfur or nitrogen than the one containing micro-sized zeolite.

  9. Copper Tetrahydrosalen Complex Encapsulated in Zeolite Y:an Effective Heterogeneous Catalyst for the Oxidation of Cycloalkanes

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    A new heterogeneous catalyst, copper tetrahydrosalen complex encapsulated in zeolite Y (denoted as Cu[H4]salen/Y) has been developed with flexible ligand method, and characterized by FTIR, DR UV-Vis spectroscopy, N2 adsorption/desorption at -196℃. This catalyst behaved like a bio-mimic enzyme, and exhibited much higher activity for the oxidation of cycloalkanes than Cusalen/Y prepared with the same method. The effects of the reaction conditions on the catalytic performance were investigated.

  10. Bayberry-like ZnO/MFI zeolite as high performance methanol-to-aromatics catalyst.

    Science.gov (United States)

    Wang, Ning; Qian, Weizhong; Shen, Kui; Su, Chang; Wei, Fei

    2016-02-01

    Unique bayberry-like MFI zeolites are synthesized through a quasi-solid-state crystallization approach. This hierarchical zeolite structure has a relatively thick shell, densely grown nanocrystals with an ordered packed channel, high mechanical stability, high surface area and a low Si/Al ratio. Its catalytic efficiency for methanol-to-aromatics is significantly higher than that of conventional MFI zeolites.

  11. Systems including catalysts in porous zeolite materials within a reactor for use in synthesizing hydrocarbons

    Science.gov (United States)

    Rolllins, Harry W [Idaho Falls, ID; Petkovic, Lucia M [Idaho Falls, ID; Ginosar, Daniel M [Idaho Falls, ID

    2012-07-24

    Catalytic structures include a catalytic material disposed within a zeolite material. The catalytic material may be capable of catalyzing a formation of methanol from carbon monoxide and/or carbon dioxide, and the zeolite material may be capable of catalyzing a formation of hydrocarbon molecules from methanol. The catalytic material may include copper and zinc oxide. The zeolite material may include a first plurality of pores substantially defined by a crystal structure of the zeolite material and a second plurality of pores dispersed throughout the zeolite material. Systems for synthesizing hydrocarbon molecules also include catalytic structures. Methods for synthesizing hydrocarbon molecules include contacting hydrogen and at least one of carbon monoxide and carbon dioxide with such catalytic structures. Catalytic structures are fabricated by forming a zeolite material at least partially around a template structure, removing the template structure, and introducing a catalytic material into the zeolite material.

  12. Transalkylation of ethyl benzene with triethylbenzene over ZSM-5 zeolite catalyst

    KAUST Repository

    Akhtar, M. Naseem

    2010-09-01

    Transalkylation of 1,3,5-triethylbenzene (TEB) with ethylbenzene (EB) has been studied over ZSM-5 zeolite using a riser simulator reactor with respect to optimizing DEB yield. The reaction temperature was varied from 350 to 500°C with contact time ranging from 3 to 15s to report on the effect of reaction conditions on TEB conversion, DEB selectivity and isomerization of TEB. The transalkylation of TEB with EB was compared with the reactions of pure 1,3,5-TEB and EB (disproportionation, isomerization and cracking). A synergistic effect was observed on the conversion of 1,3,5-TEB and DEB yield. The 1,3,5-TEB conversion increased from 40% to 50% with simultaneous increase in the DEB selectivity from 17% to 36% in transalkylation reaction (EB+1,3,5-TEB) as compared with the reaction of pure 1,3,5-TEB. It was found that pure 1,3,5-TEB underwent cracking reaction to produce DEB and EB. The isomerization of 1,3,5-TEB was more active at low temperature while cracking was more active at high temperature. The temperature of 350°C was observed as the optimum for production of maximum amount of DEB. Kinetic parameters for the disappearance of 1,3,5-TEB during its transformation reaction via cracking and isomerization pathways were calculated using the catalyst activity decay function based on time-on-stream (TOS). The apparent activation energies decrease in order E secondary cracking>E primary racking>E isomerization for ZSM-5 catalysts. © 2010 Elsevier B.V.

  13. Hydrophobic Zeolites for Applications in Adsorption and Catalysis

    OpenAIRE

    Huang, Zige; Cordon, Michael; Gounder, Rajamani

    2016-01-01

    Lewis acidic zeolites such as Sn-Beta are commonly studied for use as selective catalysts for glucose isomerization to fructose in liquid water. Glucose to fructose isomerization is a critical reaction for lignocellulosic biomass upgrading, which converts abundant and renewable feedstocks into commercially desirable fuels and chemicals. Industrial applications require catalysts that maintain optimal reactivity over long time scales, yet at typical reaction temperatures, Lewis acidic Beta z...

  14. Low-temperature activation of methane over rare earth metals promoted Zn/HZSM-5 zeolite catalysts in the presence of ethylene

    Institute of Scientific and Technical Information of China (English)

    Hengqiang Zhang; Aiguo Kong; Yongjie Ding; Chengyong Dai; Yongkui Shan

    2011-01-01

    At low temperature of 723 K, methane can be easily activated in the presence of ethylene in the feed, and converted to higher hydrocarbons (C2-C4) and aromatics (C6-C10), through its reaction over rare metals modified Zn/HZSM-5 zeolite catalysts without undesirable carbon oxides formation.Methane can get 37.3% conversion over the above catalysts under Iow temperature, and the catalysts show a longer lifetime than usual metal supported HZSM-5 zeolite catalysts without adding any rare earth metals.The effects of methane activation over various rare earth metal promoted Zn/HZSM-5 catalysts on the products and influences of several reaction conditions such as temperature, catalyst lifetime and molar ratio of CH4/C2H4 have been discussed.

  15. Zeolite H-BEA catalysed multicomponent reaction: One-pot synthesis of amidoalkyl naphthols - Biologically active drug-like molecules

    Indian Academy of Sciences (India)

    Sunil R Mistry; Rikesh S Joshi; Kalpana C Maheria

    2011-07-01

    Zeolite has been used as an efficient and a novel heterogeneous catalyst for one-pot synthesis of biologically active drug-like molecules, amidoalkyl naphthols. This green route involves multicomponent reaction of 2-naphthol, aromatic aldehydes and amide in the presence of a catalytic amount of zeolite H-Beta (H-BEA) under solvent reflux as well as solvent-free conditions.

  16. Inlfuence of the Alkali Treatment of HZSM-5 Zeolite on Catalytic Performance of PtSn-Based Catalyst for Propane Dehydrogenation

    Institute of Scientific and Technical Information of China (English)

    Huang Li; Zhou Shijian; Zhou Yuming; Zhang Yiwei; Xu Jun; Wang Li

    2013-01-01

    The porous material ATZ with micro-mesopore hierarchical porosity was prepared by alkali treatment of parent HZSM-5 zeolite and applied for propane dehydrogenation. The zeolite samples were characterized by XRD, N2-physisorption, and NH3-TPD analysis. The results showed that the alkali treatment can modify the physicochemical prop-erties of HZSM-5 zeolite. In this case, the porous material ATZ showed larger external surface area with less acid sites as compared to the HZSM-5 zeolite. It was found out that the alkali treatment of HZSM-5 zeolite could promote the catalytic performance of PtSn/ATZ catalyst. The possible reason was ascribed to the low acidity of ATZ. Furthermore, the presence of mesopores could reduce the carbon deposits on the metallic surface, which was also favorable for the dehydrogenation reaction.

  17. Fully Copper-Exchanged High-Silica LTA Zeolites as Unrivaled Hydrothermally Stable NH3 -SCR Catalysts.

    Science.gov (United States)

    Ryu, Taekyung; Ahn, Nak Ho; Seo, Seungwan; Cho, Jung; Kim, Hyojun; Jo, Donghui; Park, Gi Tae; Kim, Pyung Soon; Kim, Chang Hwan; Bruce, Elliott L; Wright, Paul A; Nam, In-Sik; Hong, Suk Bong

    2017-03-13

    Diesel engine technology is still the most effective solution to meet tighter CO2 regulations in the mobility and transport sector. In implementation of fuel-efficient diesel engines, the poor thermal durability of lean nitrogen oxides (NOx ) aftertreatment systems remains as one major technical hurdle. Divalent copper ions when fully exchanged into high-silica LTA zeolites are demonstrated to exhibit excellent activity maintenance for NOx reduction with NH3 under vehicle simulated conditions even after hydrothermal aging at 900 °C, a critical temperature that the current commercial Cu-SSZ-13 catalyst cannot overcome owing to thermal deactivation. Detailed structural characterizations confirm the presence of Cu(2+) ions only at the center of single 6-rings that act not only as a catalytically active center, but also as a dealumination suppressor. The overall results render the copper-exchanged LTA zeolite attractive as a viable substitute for Cu-SSZ-13.

  18. Designing zeolite catalysts for size- and shape-selective reactions: Selective hydrogenation of acetylene in the presence of butadiene and ethylene

    Energy Technology Data Exchange (ETDEWEB)

    Corbin, D.R.; Abrams, L.; Bonifaz, C. (E.I. du Pont de Nemours Company, Wilmington, DE (USA))

    1989-02-01

    In the production of ethylene from the steam cracking of natural gas, small amounts of acetylene and butadiene are produced. Downstream, acetylene can present a hazard in a cryogenic separation process while nonselective hydrogenation removes acetylene as well as valuable ethylene and butadiene. With the aid of adsorption measurements, a selective hydrogenation catalyst has been designed. Small-pore zeolites, which serve as catalytic supports and provide reactant selective control, were ion-exchanged with Ni{sup 2+} and subsequently reduced. Compared to a commercial catalyst in which 60% of butadiene and all of the acetylene are hydrogenated, these new catalysts totally hydrogenate acetylene with only 10-20% hydrogenation of the butadiene and almost no hydrogenation of ethylene. To achieve selective hydrogenation, poisoning of the metal sites on the external zeolite surface is essential in order to obtain a product spectrum dominated by catalytic sites within the zeolite framework.

  19. Intergrown new zeolite beta polymorphs with interconnected 12-ring channels solved by combining electron crystallography and single-crystal X-ray diffraction

    KAUST Repository

    Yu, Zhengbao

    2012-10-09

    Two new polymorphs of zeolite beta, denoted as SU-78A and SU-78B, were synthesized by employing dicyclohexylammonium hydroxides as organic structure-directing agents. The structure was solved by combining transmission electron microscopy and single-crystal X-ray diffraction. SU-78 is an intergrowth of SU-78A and SU-78B and contains interconnected 12-ring channels in three directions. The two polymorphs are built from the same building layer, similar to that for the zeolite beta family. The layer stacking in SU-78, however, is different from those in zeolite beta polymorph A, B, and C, showing new zeolite framework topologies. SU-78 is thermally stable up to 600 °C. © 2012 American Chemical Society.

  20. Features of non-oxidative conversion of methane into aromatic hydrocarbons over Mo-containing zeolite catalysts

    Science.gov (United States)

    Stepanov, A. A.; Korobitsyna, L. L.; Vosmerikov, A. V.

    2016-09-01

    The results of study of methane conversion under non-oxidative conditions over molybdenum containing zeolite catalysts prepared by solid-phase synthesis using nanosized molybdenum powder are presented. The kinetic mechanisms of the process behavior under different conditions of methane dehydroaromatization are determined. It is shown that nonoxidative conversion of methane can occur both in the external diffusion and kinetic regions, depending on the methane flow rate. It is found out, that the optimum temperature of the methane conversion is 750 °C. It is shown that increased methane conversion is observed at the feed space velocity of methane decreasing from 1500 to 500 h-1.

  1. XAFS study on active Pr sites in zeolite as a photo catalyst for decomposition of nitrous oxide

    Energy Technology Data Exchange (ETDEWEB)

    Ebitani, Kohki; Mizugaki, Tomoo; Kaneda, Kiyotomi [Osaka Univ., Graduate School of Engineering Science, Osaka (Japan); Nishi, Akio; Hirano, Yoshiaki [Tokyo Inst. of Technology, Graduate School of Science and Engineering, Tokyo (Japan); Yoshida, Hisao [Nagoya Univ., Graduate School of Engineering, Nagoya (Japan); Tanaka, Tsunehiro [Kyoto Univ., Graduate School of Engineering, Kyoto (Japan); Morikawa, Akira [Shinshu Univ., Faculty of Textile Science and Technology, Dept. of Kansei Engineering, Ueda (Japan)

    2001-03-01

    The praseodymium-exchanged mordenite degassed at 873 K acted as a highly active heterogeneous photo catalyst for the stoichiometric decomposition of N{sub 2}O. Analysis of Pr L{sub 3}-edge EXAFS revealed that the Pr species were isolated each other in the large channel of zeolite, and that the active Pr species were coordinated by ca. four oxygen atoms and one Al atom. On the other hands, the inactive Pr species are surrounded by ca. 10 oxygens of adsorbed waters. The former low-coordinated Pr species allowed a strong adsorption of N{sub 2}O, which could be the first step of the decomposition reaction. (au)

  2. Acidic and basic properties of zeolite-containing cracking catalyst in the process of butene-1 isomerization

    Science.gov (United States)

    Mursalova, L. A.; Guseinova, E. A.; Adzhamov, K. Yu.

    2016-08-01

    The process of butene-1 isomerization in the presence of two groups of samples of zeolite-containing catalyst (ZCC) that earlier participated in the traditional and oxidative catalytic cracking of vacuum gasoil is investigated. It is established that the nature of the reaction mixture and conditions of the cracking process are key factors in forming the acidic and basic properties of the catalyst. It is shown that the highest activity in the butene-1 isomerization into cis-/ trans-butene-2 is demonstrated by ZCC samples that participated in the oxidative catalytic cracking (oxycracking). It is suggested that the enhanced catalytic activity of this group of ZCC samples was related to the availability of acid-base centers in the form of radical-like oxygen along with protic- and aprotic-type acidic centers in the structure of the oxidative compaction products.

  3. ZEOLITES: EFFECTIVE WATER PURIFIERS

    Science.gov (United States)

    Zeolites are known for their adsorption, ion exchange and catalytic properties. Various natural zeolites are used as odor and moisture adsorbents and water softeners. Due to their acidic nature, synthetic zeolites are commonly employed as solid acid catalysts in petrochemical ind...

  4. Effect of combining the metals of group VI supported on H-ZSM-5 zeolite as catalysts for non-oxidative conversion of natural gas to petrochemicals

    Institute of Scientific and Technical Information of China (English)

    A.K.Aboul-Gheit; A.E.Awadallah

    2009-01-01

    The most prestigious catalyst applied in natural gas (methane) non-oxidative conversion to petrochemicals is 6%Mo/H-ZSM-5.Chromium,molybdenum and tungsten are the group VI metals.Hence,in this work,6%Mo/H-ZSM-5 was correlated with 3%Cr+3%Mo/H-ZSM-5 and 3%W+3%Mo/H-ZSM-5 as catalysts to examine their promoting or inhibiting effects on the various reactions taking place during methane conversion.The catalytic activities of these catalysts were tested in a continuous flow fixed bed reactor at 700℃ and a GHSV of 1500 ml·g-1 ·h-1. Characterization of the catalysts using XRD,TGA and TPD were investigated.XRD and NH3-TPD showed greater interaction between the W-phase and the Bronsted acid sites in the channels of the zeolite than between Cr-phase and the acid sites in the zeolite.

  5. Capture and isotopic exchange method for water and hydrogen isotopes on zeolite catalysts up to technical scale for pre-study of processing highly tritiated water

    Energy Technology Data Exchange (ETDEWEB)

    Michling, R.; Braun, A.; Cristescu, I.; Dittrich, H.; Gramlich, N.; Lohr, N. [Karlsruhe Institute of Technology, Eggenstein-Leopoldshafen (Germany); Glugla, M.; Shu, W.; Willms, S. [ITER Organization, Saint-Paul-lez-Durance (France)

    2015-03-15

    Highly tritiated water (HTW) may be generated at ITER by various processes and, due to the excessive radio toxicity, the self-radiolysis and the exceedingly corrosive property of HTW, a potential hazard is associated with its storage and process. Therefore, the capture and exchange method for HTW utilizing Molecular Sieve Beds (MSB) was investigated in view of adsorption capacity, isotopic exchange performance and process parameters. For the MSB, different types of zeolite were selected. All zeolite materials were additionally coated with platinum. The following work comprised the selection of the most efficient zeolite candidate based on detailed parametric studies during the H{sub 2}/D{sub 2}O laboratory scale exchange experiments (about 25 g zeolite per bed) at the Tritium Laboratory Karlsruhe (TLK). For the zeolite, characterization analytical techniques such as Infrared Spectroscopy, Thermogravimetry and online mass spectrometry were implemented. Followed by further investigation of the selected zeolite catalyst under full technical operation, a MSB (about 22 kg zeolite) was processed with hydrogen flow rates up to 60 mol*h{sup -1} and deuterated water loads up to 1.6 kg in view of later ITER processing of arising HTW. (authors)

  6. Structural Descriptors of Zeolitic-Imidazolate Frameworks Are Keys to the Activity of Fe-N-C Catalysts.

    Science.gov (United States)

    Armel, Vanessa; Hindocha, Sheena; Salles, Fabrice; Bennett, Stephen; Jones, Deborah; Jaouen, Frédéric

    2017-01-11

    Active and inexpensive catalysts for oxygen reduction are crucially needed for the widespread development of polymer electrolyte fuel cells and metal-air batteries. While iron-nitrogen-carbon materials pyrolytically prepared from ZIF-8, a specific zeolitic imidazolate framework (ZIF) with sodalite topology, have shown enhanced activities toward oxygen reduction in acidic electrolyte, the rational design of sacrificial metal-organic frameworks toward this application has hitherto remained elusive. Here, we report for the first time that the oxygen reduction activity of Fe-N-C catalysts positively correlates with the cavity size and mass-specific pore volume in pristine ZIFs. The high activity of Fe-N-C materials prepared from ZIF-8 could be rationalized, and another ZIF structure leading to even higher activity was identified. In contrast, the ORR activity is mostly unaffected by the ligand chemistry in pristine ZIFs. These structure-property relationships will help identifying novel sacrificial ZIF or porous metal-organic frameworks leading to even more active Fe-N-C catalysts. The findings are of great interest for a broader application of the class of inexpensive metal-nitrogen-carbon catalysts that have shown promising activity also for the hydrogen evolution (Co-N-C) and carbon dioxide reduction (Fe-N-C and Mn-N-C).

  7. Selective Chemical Conversion of Sugars in Aqueous Solutions without Alkali to Lactic Acid Over a Zn-Sn-Beta Lewis Acid-Base Catalyst

    Science.gov (United States)

    Dong, Wenjie; Shen, Zheng; Peng, Boyu; Gu, Minyan; Zhou, Xuefei; Xiang, Bo; Zhang, Yalei

    2016-05-01

    Lactic acid is an important platform molecule in the synthesis of a wide range of chemicals. However, in aqueous solutions without alkali, its efficient preparation via the direct catalysis of sugars is hindered by a side dehydration reaction to 5-hydroxymethylfurfural due to Brønsted acid, which originates from organic acids. Herein, we report that a previously unappreciated combination of common two metal mixed catalyst (Zn-Sn-Beta) prepared via solid-state ion exchange synergistically promoted this reaction. In water without a base, a conversion exceeding 99% for sucrose with a lactic acid yield of 54% was achieved within 2 hours at 190 °C under ambient air pressure. Studies of the acid and base properties of the Zn-Sn-Beta zeolite suggest that the introduction of Zn into the Sn-Beta zeolite sequentially enhanced both the Lewis acid and base sites, and the base sites inhibited a series of side reactions related to fructose dehydration to 5-hydroxymethylfurfural and its subsequent decomposition.

  8. Improved Automotive NO (x) Aftertreatment System: Metal Ammine Complexes as NH3 Source for SCR Using Fe-Containing Zeolite Catalysts

    DEFF Research Database (Denmark)

    Johannessen, Tue; Schmidt, Henning; Frey, Anne Mette

    2009-01-01

    Ammonia storage is a challenge in the selective catalytic reduction of NO (x) in vehicles. We propose a new system, based on metal ammines as the ammonia source. In combination with iron containing zeolites as the SCR catalyst it should be possible to obtain a low temperature system for NO (x...

  9. Indole cyanation via C-H bond activation under catalysis of Ru(Ⅲ)-exchanged NaY zeolite (RuY) as a recyclable catalyst

    Institute of Scientific and Technical Information of China (English)

    Alireza Khorshidi

    2012-01-01

    Selective 3-cyanation of indoles was achieved under heterogeneous catalysis of Ru(Ⅲ)-exchanged NaY zeolite (RuY) as a recyclable catalyst,in combination with K4[Fe(CN)6] as a nontoxic,slow cyanide releasing agent.Under the aforementioned conditions,good yields of the desired products were obtained.

  10. CHARACTERIZATION OF H-Y AND CR-Y ZEOLITE CATALYSTS DURING THE OXIDATIVE DESTRUCTION OF CFC11 AND CFC12

    Science.gov (United States)

    The long term stability-deactivation characteristics of two Y zeolite catalysts, namely H-Y and cation exchanged Cr-Y, were studied during the oxidative destruction of CFC11 and CFC12 feeds. Experiments were carried out at 300 degrees C and 500 h-1 space velocity. Properties of...

  11. Zeolite (ZSM-5 as a Highly Efficient and Heterogeneous Catalyst for the Synthesis of β-Enaminones and β-Enamino Esters

    Directory of Open Access Journals (Sweden)

    Amiya Shekhar

    2011-01-01

    Full Text Available Several β-enaminones and β-enaminoesters have been synthesized in high yields from amine and β-diketone in the presence of Zeolite (ZSM-5 as a catalyst. This method is applicable to both cyclic and acyclic ketones with aromatic and aliphatic amines.

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

    Science.gov (United States)

    Widayat, Widayat; Roesyadi, A.; Rachimoellah, M.

    2009-09-01

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

  13. An electrode with Ni(II) loaded analcime zeolite catalyst for the electrooxidation of methanol

    Institute of Scientific and Technical Information of China (English)

    Seyed Naser Azizi; Shahram Ghasemi; Neda Salek Gilani

    2014-01-01

    There is a high overvoltage in the oxidation of methanol in fuel cells, and so modified electrodes are used to decrease it. A modified electrode that used Ni(II) loaded analcime zeolite to catalyze the electrooxidation of methanol in alkaline solution was proposed. Analcime zeolite was synthesized by hydrothermal synthesis, and Ni(II) ions were incorporated into the analcime structure, which was then mixed with carbon paste to prepare modified electrode. The electrocatalytic oxidation of methanol on the surface of the modified electrode in alkaline solution was investigated by cyclic voltammetry and chronoamperometry. The effects of the scan rate of the potential, concentration of methanol, and amount of zeolite were investigated. The rate constant for the catalytic reaction of methanol was 6 × 103 cm3 mol-1 s-1 from measurements using chronoamperometry. The proposed electrode significantly improved the electron transfer rate and decreased the overpotential for methanol oxidation.

  14. S +X-I + route to mesostructured materials from Fau and Beta zeolite precursors: A comparative study of their assembly behaviors in extremely acidic media

    Science.gov (United States)

    Zheng, Junlin; Zhai, Shangru; Wu, Dong; Sun, Yuhan

    2005-05-01

    Mesoporous molecular sieves were synthesized from Beta and Fau zeolite precursors through S +X-I + route under extremely acidic conditions in parallel (designated as MBeta and MFau, respectively). The textural properties of MFau were different from its MBeta counterpart but resembled normal MCM-41 silica from TEOS. Al content in MBeta was almost equivalent to that in the initial Beta zeolite precursors, whereas only trace Al species was present in MFau from elemental analysis results. The hydrothermal stability of MBeta after post-synthesis ammonia treatment was considerably improved compared with normal MCM-41 aluminosilicates, whereas the MFau after the same procedure was as unstable as normal MCM-41 silica. Thus, the assembly behaviors of Beta and Fau zeolite precursors were comparatively studied based on these results. The microstructure of Fau zeolite precursors were degraded by the extremely acidic condition, and Al species was dissolved into the synthesis mixture. However, Beta zeolite precursors survived the chemical attack of extremely acidic media and were incorporated into mesostructured framework as primary building units.

  15. Synthesis of mesoporous zeolite catalysts by in situ formation of carbon template over nickel nanoparticles

    DEFF Research Database (Denmark)

    Abildstrøm, Jacob Oskar; Kegnæs, Marina; Hytoft, Glen

    2016-01-01

    A novel synthesis procedure for the preparation of the hierarchical zeolite materials with MFI structure based on the carbon templating method with in situ generated carbon template is presented in this study. Through chemical vapour deposition of coke on nickel nanoparticles supported on silica...... oxide, a carbon-silica composite is obtained and exploited as a combined carbon template/silica source for zeolite synthesis. This approach has several advantages in comparison with conventional carbon templating methods, where relatively complicated preparative strategies involving multistep...

  16. Photocatalytic oxidation of NO{sub x} over TiO{sub 2}/HZSM-5 catalysts in the presence of water vapor: Effect of hydrophobicity of zeolites

    Energy Technology Data Exchange (ETDEWEB)

    Guo, Gaofei [The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, College of Environmental Science and Engineering, South China University of Technology, Guangzhou 510006 (China); Hu, Yun, E-mail: huyun@scut.edu.cn [The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, College of Environmental Science and Engineering, South China University of Technology, Guangzhou 510006 (China); Jiang, Shumei; Wei, Chaohai [The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, College of Environmental Science and Engineering, South China University of Technology, Guangzhou 510006 (China)

    2012-07-15

    Highlights: Black-Right-Pointing-Pointer The photooxidation of NO{sub x} over TiO{sub 2}/HZSM-5 was tested in the presence of water vapor. Black-Right-Pointing-Pointer TiO{sub 2}/HZSM-5 exhibited higher NO conversion and lower NO{sub 2} formation than pure TiO{sub 2}. Black-Right-Pointing-Pointer Water vapor related to relative humidity and water pre-adsorption was effect factor. Black-Right-Pointing-Pointer TiO{sub 2} hybridized with hydrophobic HZSM-5 zeolite retained high reactivity. Black-Right-Pointing-Pointer Photocatalytic reactivity of TiO{sub 2}/HZSM-5 depended on hydrophobicity of zeolites. - Abstract: TiO{sub 2} hybridized with HZSM-5 zeolites photocatalysts were prepared by a simple solid state dispersion method. The physicochemical properties of the catalysts were characterized by X-ray diffraction, UV-vis diffuse reflectance and FT-IR spectroscopy. The photocatalytic oxidation of NO{sub x} over TiO{sub 2}/HZSM-5 having different Si/Al ratios was carried out under various levels of humidity and different pre-adsorption times in dark. The TiO{sub 2}/HZSM-5 composite catalysts exhibited higher NO conversion and lower NO{sub 2} formation than pure TiO{sub 2}. Pre-adsorption with water vapor and the high humidity during the photoreaction were harmful to the reactivity of TiO{sub 2} hybridized with hydrophilic HZSM-5 zeolite. However, the photocatalytic reactivity of TiO{sub 2} hybridized with hydrophobic zeolite varied little with increase in humidity. The results indicated that the high photocatalytic reactivity of TiO{sub 2}/HZSM-5 catalysts is largely depended on the hydrophobicity of the zeolites.

  17. 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.

  18. SYNTHESIS OF ZEOLITE SOCONY MOBIL FROM BLUE SILICA GEL AND RICE HUSK ASH AS CATALYSTS FOR HYDROTHERMAL LIQUEFACTION

    Directory of Open Access Journals (Sweden)

    SUYITNO

    2015-08-01

    Full Text Available Renewable biofuels produced by the hydrothermal liquefaction of rice husks have received much attention because of rapid increases in fuel consumption and corresponding declines in fossil fuel resources. To increase biofuel yields, template-free syntheses of Zeolite Socony Mobil (ZSM catalysts based on blue silica gel and rice husk ash as silica sources were studied. After ZSM synthesis in a closed reactor at 170°C, the crystallinity and crystalline diameters of the products were determined by X-ray diffraction, affording values of 56.33%– 65.81% and 64.3–68.5 nm, respectively. The hydrothermal liquefaction of rice husks with or without a catalyst was conducted in a closed reactor (1200 mm length × 100 mm diameter at 275°C for 45 min. The light biofuel was separated from the ethanol solvent and heavy biofuel via vacuum evaporation. The ZSM catalysts increased the biofuel yields by 2.9%–6.0%. The light biofuels exhibited heating values, flash points, and viscosities of approximately 4.2–4.3 kcal·g−1, 19°C, and 1.48–1.52 cSt, respectively. However, further studies are required to enhance the activity of the ZSMs and increase the quality of the biofuels.

  19. Investigation of PCDD/F emissions from mobile source diesel engines: impact of copper zeolite SCR catalysts and exhaust aftertreatment configurations.

    Science.gov (United States)

    Liu, Z Gerald; Wall, John C; Barge, Patrick; Dettmann, Melissa E; Ottinger, Nathan A

    2011-04-01

    This study investigated the impact of copper zeolite selective catalytic reduction (SCR) catalysts and exhaust aftertreatment configurations on the emissions of polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) from mobile source diesel engines. Emissions of PCDD/Fs, reported as the weighted sum of 17 congeners called the toxic equivalency quotient (TEQ), were measured using a modified EPA Method 0023A in the absence and presence of exhaust aftertreatment. Engine-out emissions were measured as a reference, while aftertreatment configurations included various combinations of diesel oxidation catalyst (DOC), diesel particulate filter (DPF), Cu-zeolite SCR, Fe-zeolite SCR, ammonia oxidation catalyst (AMOX), and aqueous urea dosing. In addition, different chlorine concentrations were evaluated. Results showed that all aftertreatment configurations reduced PCDD/F emissions in comparison to the engine-out reference, consistent with reduction mechanisms such as thermal decomposition or combined trapping and hydrogenolysis reported in the literature. Similarly low PCDD/F emissions from the DOC-DPF and the DOC-DPF-SCR configurations indicated that PCDD/F reduction primarily occurred in the DOC-DPF with no noticeable contribution from either the Cu- or Fe-zeolite SCR systems. Furthermore, experiments performed with high chlorine concentration provided no evidence that chlorine content has an impact on the catalytic synthesis of PCDD/Fs for the chlorine levels investigated in this study.

  20. Easily recoverable titanosilicate zeolite beads with hierarchical porosity: Preparation and application as oxidation catalysts

    NARCIS (Netherlands)

    Cheng, Wenjing; Jiang, Yanqiu; Xu, Xianzhu; Wang, Yan; Lin, Kaifeng; Pescarmona, Paolo P.

    2016-01-01

    Titanosilicate zeolite beads with hierarchical porosity and 0.2-0.5 mm diameter (HPB-TS-1) have been synthesized from a titanosilicate solution, employing a porous anion-exchange resin as shape- and structure-directing template. The characterization results showed the existence of crystalline TS-1 n

  1. Kinetic-Thermodynamic Analysis of the Reactive Distillation Process of the Cyclohexene Hydration Using the Zeolite Catalyst

    Institute of Scientific and Technical Information of China (English)

    叶建初; 黄佳丽; 林晗丹; 曹克腾; 沙勇

    2011-01-01

    Reactive distillation could be utilized to produce cyclohexanol through the cyclohexene hydration. By means of highly active zeolite catalyst HZSM-5, the kinetic-thermodynamic analysis of this reactive distillation has been carried out to get the characteristics of the reactive distillation. Results from kinetic and thermodynamic analysis indicate that the optimal pressure of this reactive distillation process should be set to higher pressure such as 0.3 or 0.4 MPa. To avoid the recovery of cyclohexanol at the top of the column, an unreactive section should be allocated at the upper column. In addition, the inert component benzene is more unfavorable to the reactive distillation process in comparison with the inert cyclohexane.

  2. Synthesis of Fatty Alcohols from Oil Palm Using a Catalyst of Ni-Cu Supported onto Zeolite

    Directory of Open Access Journals (Sweden)

    L. Giraldo

    2010-01-01

    Full Text Available A series of Ni-Cu supported onto zeolite type ZSM-5 has been synthesized by direct hydrothermal method without template agent and characterized using XRD, FT-IR, NRM mass, SEM, CG and N2 adsorption techniques. The catalytic performance of the obtained materials was evaluated and utilized for the hydrogenation of palm oil at 453 K and 40 atmospheres of pressure. The results show that the samples exhibited typical hexagonal arrangement of mesoporous structure with high surface area and the heteroatoms were probably incorporated into the framework of ZSM-5. Catalytic tests show that the bimetallic incorporated materials were effective as catalysts in the hydrogenation of oil palm producing fatty alcohols typical.

  3. Hydroisomerization of n-heptane over bimetal-bearing H3PW12O40 catalysts supported on dealuminated USY zeolite

    Institute of Scientific and Technical Information of China (English)

    WEI RuiPing; GU YanBo; WANG Jun

    2008-01-01

    The bimetal-bearing (CePt or LaPt) 12-tungstophosphoric acid (H3PW12O40 (PW)) catalysts supported on dealuminated USY zeolite (DUSY) were prepared by impregnation and characterized by XRD, BET, IR, and H2-chemisorption.Their catalytic activities were tested in the hydroisomerization of n-heptane with a continuous atmospheric fixed-bed reactor.After the steam treatment combined with the acid leaching, as well as the supporting with PW and the bimetals, the DUSY support retains the Y zeolite porosity and the PW well keeps its Keggin structure in catalysts.The doping of Ce into the catalysts enhances the dispersion of Pt on the catalyst surface.The Pt-bearing PW catalysts doped with Ce or La, especially Ce, exhibit much higher catalytic activity and selectivity than the catalysts without dopants at lowered re-action temperatures.At the optimal reaction conditions, i.e., the reaction temperature of 250℃ and WHSV of 1.4 h-1, the catalyst with a Pt loading of 0.4%, PW loading of 10% and a molar ratio of Ce to Pt of 15:1 shows a conversion of n-heptane of 70.3% with a high selectivity for isomerization products of 94.1%.

  4. Hydroisomerization of n-heptane over bimetal-bearing H3PW12O40 catalysts supported on dealuminated USY zeolite

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    The bimetal-bearing (CePt or LaPt) 12-tungstophosphoric acid (H3PW12O40 (PW)) catalysts supported on dealuminated USY zeolite (DUSY) were prepared by impregnation and characterized by XRD, BET, IR, and H2-chemisorption. Their catalytic activities were tested in the hydroisomerization of n-heptane with a continuous atmospheric fixed-bed reactor. After the steam treatment combined with the acid leaching, as well as the supporting with PW and the bimetals, the DUSY support retains the Y zeolite porosity and the PW well keeps its Keggin structure in catalysts. The doping of Ce into the catalysts enhances the dispersion of Pt on the catalyst surface. The Pt-bearing PW catalysts doped with Ce or La, especially Ce, exhibit much higher catalytic activity and selectivity than the catalysts without dopants at lowered reaction temperatures. At the optimal reaction conditions, i.e., the reaction temperature of 250℃ and WHSV of 1.4 h1, the catalyst with a Pt loading of 0.4%, PW loading of 10% and a molar ratio of Ce to Pt of 15:1 shows a conversion of n-heptane of 70.3% with a high selectivity for isomerization products of 94.1%.

  5. Catalytic Dehydration of Glycerol to Acrolein over a Catalyst of Pd/LaY Zeolite and Comparison with the Chemical Equilibrium

    Directory of Open Access Journals (Sweden)

    Israel Pala Rosas

    2017-02-01

    Full Text Available Glycerol dehydration to acrolein was studied with three catalysts using zeolite-Y. This zeolite in its protonic form (HY, with La (LaY and Pd with La (Pd/LaY, was characterized by X-ray diffraction (XRD, Fourier-transform-infrared spectroscopy (FTIR with pyridine, BET, Scanning Electron Microscope (SEM–Energy-Dispersive Spectroscopy X-ray (EDS and the catalytic activity tests were carried out under H2 atmosphere. It was found that La ions exchanged in the zeolite-Y resulted in the improvement of both glycerol conversion and yield to acrolein, also a relatively constant glycerol conversion was achieved up to three hours, due to the presence of Pd on the catalyst and H2 in the feed. The comparison of the calculated and experimental yields obtained from the catalytic tests of the Pd/LaY catalyst indicates a greater activity for the reaction to acrolein than for the reaction to acetol. The calculated equilibrium yields of the dehydration reaction from glycerol to acrolein, acetol, ethanal, methanol, and water and the experimental yields of a Pd/LaY catalyst were compared. Thermodynamically, a complete conversion of glycerol can be achieved since the general system remains exothermic and promotes the path to acetol below 480 K. Above this temperature the system consumes energy and favors the production of acrolein, reaching its maximum concentration at 600 K.

  6. HERFD-XANES and XES as complementary operando tools for monitoring the structure of Cu-based zeolite catalysts during NOx-removal by ammonia SCR

    Science.gov (United States)

    Günter, T.; Doronkin, D. E.; Carvalho, H. W. P.; Casapu, M.; Grunwaldt, J.-D.

    2016-05-01

    In this article, we demonstrate the potential of hard X-ray techniques to characterize catalysts under working conditions. Operando high energy resolution fluorescence detected (HERFD) XANES and valence to core (vtc) X-ray emission spectroscopy (XES) have been used in a spatially-resolved manner to study Cu-zeolite catalysts during the standard-SCR reaction and related model conditions. The results show a gradient in Cu oxidation state and coordination along the catalyst bed as the reactants are consumed. Vtc-XES gives complementary information on the direct adsorption of ammonia at the Cu sites. The structural information on the catalyst shows the suitability of X-ray techniques to understand catalytic reactions and to facilitate catalyst optimization.

  7. Titanium-Beta Zeolites Catalyze the Stereospecific Isomerization of D-Glucose to L-Sorbose via Intramolecular C5-C1 Hydride Shift

    Energy Technology Data Exchange (ETDEWEB)

    Gounder, Rajamani [California Inst. of Technology (CalTech), Pasadena, CA (United States); Davis, Mark E. [California Inst. of Technology (CalTech), Pasadena, CA (United States)

    2013-06-03

    Pure-silica zeolite beta containing Lewis acidic framework Ti4+ centers (Ti-Beta) is shown to catalyze the isomerization of D-glucose to L-sorbose via an intramolecular C5–C1 hydride shift. Glucose–sorbose isomerization occurs in parallel to glucose–fructose isomerization on Ti-Beta in both water and methanol solvents, with fructose formed as the predominant product in water and sorbose as the predominant product in methanol (at 373 K) at initial times and over the course of >10 turnovers. Isotopic tracer studies demonstrate that 13C and D labels placed respectively at the C1 and C2 positions of glucose are retained respectively at the C6 and C5 positions of sorbose, consistent with its formation via an intramolecular C5–C1 hydride shift isomerization mechanism. This direct Lewis acid-mediated pathway for glucose–sorbose isomerization appears to be unprecedented among heterogeneous or biological catalysts and sharply contrasts indirect base-mediated glucose–sorbose isomerization via 3,4-enediol intermediates or via retro-aldol fragmentation and recombination of sugar fragments. Measured first-order glucose–sorbose isomerization rate constants (per total Ti; 373 K) for Ti-Beta in methanol are similar for glucose and glucose deuterated at the C2 position (within a factor of ~1.1), but are a factor of ~2.3 lower for glucose deuterated at each carbon position, leading to H/D kinetic isotope effects expected for kinetically relevant intramolecular C5–C1 hydride shift steps. Optical rotation measurements show that isomerization of D-(+)-glucose (92% enantiomeric purity) with Ti-Beta in water (373 K) led to the formation of L-(-)-sorbose (73% enantiomeric purity) and D-(-)-fructose (87% enantiomeric purity) as the predominant stereoisomers, indicating that stereochemistry is preserved at carbon centers not directly involved in intramolecular C5–C1 or C2–C1 hydride shift steps, respectively. This new Lewis acid

  8. [EMIM]Br中H-Beta沸石催化蔗糖脱水制5-羟甲基糠醛%Catalytic Dehydration of Sucrose Into 5-Hydroxymethylfurfural Over H-Beta Zeolite in [EMIM]Br

    Institute of Scientific and Technical Information of China (English)

    邱金丽; 刘民; 施金亮; 郭新闻

    2012-01-01

    In the compounded solvent of DMA and [EMIM]Br, H-Beta zeolite was employed as a catalyst to investigate its performance of catalytically converting sucrose into 5-hydroxymethylfurfural (HMF). Cr-Beta was synthesized by an ion-exchange approach with H-Beta as a suitable precursor. The catalysts were characterized by XRD, FT-IR and UV-Vis, and employed in sucrose conversion to test their catalytic performance. The results showed that a yield of 68. 3% HMF was obtained in the reaction system with m(DMA) :m([EMIMJBr) = m(Sucrose): m(Cr-Beta) = 100:12: 10: 9, reaction temperature 130℃, reaction time 90 min. Under the optimized reaction conditions, Cr-Beta showed a good reusability.%采用N,N-二甲基乙酰胺(DMA)与溴化1-乙基-3-甲基咪唑([EMlM]Br)为混合溶剂,考察了H-Beta分子筛催化蔗糖转化制5-羟甲基糠醛(HMF)反应的性能;以H-Beta分子筛为母体,离子交换法制得Cr-Beta催化剂,并采用XRD、FT-IR和UV-Vis对催化剂进行了表征,同时进行了反应性能的评价.结果表明,在DMA与[EMIM]Br混合溶剂中,当反应温度130℃、反应时间90 min、m(DMA):m([EMIM]Br):m(Sucrose):m(Cr-Beta)=100:12:10:9时,HMF的收率可达68.3%; Cr-Beta催化剂在优化的反应条件下具有良好的重复使用性能.

  9. Acid-Base Pairs in Lewis Acidic Zeolites Promote Direct Aldol Reactions by Soft Enolization.

    Science.gov (United States)

    Lewis, Jennifer D; Van de Vyver, Stijn; Román-Leshkov, Yuriy

    2015-08-17

    Hf-, Sn-, and Zr-Beta zeolites catalyze the cross-aldol condensation of aromatic aldehydes with acetone under mild reaction conditions with near quantitative yields. NMR studies with isotopically labeled molecules confirm that acid-base pairs in the Si-O-M framework ensemble promote soft enolization through α-proton abstraction. The Lewis acidic zeolites maintain activity in the presence of water and, unlike traditional base catalysts, in acidic solutions.

  10. Metal supported on natural zeolite as catalysts for conversion of ethanol to gasoline

    Directory of Open Access Journals (Sweden)

    Kristiani Anis

    2017-01-01

    Full Text Available A various of metal supported into natural zeolite was prepared via wet impregnation method. The transition metals impregnated are nickel, cobalt, copper and zinc. The catalytic properties both of physical and chemical properties were characterized by X-ray Diffraction (XRD, Thermo Gravimetri Analysis (TGA-Differential Scanning Calorimetry (DSC, Surface Area Analyzer-Porositymeter and also gravimetry method for acidity measurement following by the adsorption of organic bases. The results showed that different metals impregnated into natural zeolite affected physical and chemical properties, i.e. crystalinity, surface area, pore size, pore volume and acidity. Their catalytic activity was tested for conversion ethanol to gasoline and showed high conversion up to 80-90% with the aromatics as major product.

  11. Rapid synthesis of ZSM-5 zeolite catalyst for amination of ethanolamine

    Institute of Scientific and Technical Information of China (English)

    华月明; 胡望明

    2004-01-01

    ZSM-5 zeolite was rapidly synthesized in system containing ethylenediamine from the initial gel: (5-8) Na2O:44 EDA:A12O3:100 SiO2:4000 H2O. The crystals were lath-shaped. The effect of pretreatment and alkalinity on crystallinity was investigated. The pretreatment of silicate source can cut down the crystallization time. Tuning the system alkalinity and controlling crystallization time can ensure forming of pure crystal.

  12. Rapid synthesis of ZSM-5 zeolite catalyst for amination of ethanolamine

    Institute of Scientific and Technical Information of China (English)

    华月明; 胡望明

    2004-01-01

    ZSM-5 zeolite was rapidly synthesized in system containing ethylenediamine from the initial gel: (5(8) Na2O: 44 EDA:Al2O3:100 SiO2:4000 H2O. The crystals were lath-shaped. The effect of pretreatment and alkalinity on crystallinity was investigated. The pretreatment of silicate source can cut down the crystallization time. Tuning the system alkalinity and controlling crystallization time can ensure forming of pure crystal.

  13. Catalytic Intermediate Pyrolysis of Napier Grass in a Fixed Bed Reactor with ZSM-5, HZSM-5 and Zinc-Exchanged Zeolite-A as the Catalyst

    Directory of Open Access Journals (Sweden)

    Isah Yakub Mohammed

    2016-03-01

    Full Text Available The environmental impact from the use of fossil fuel cum depletion of the known fossil oil reserves has led to increasing interest in liquid biofuels made from renewable biomass. This study presents the first experimental report on the catalytic pyrolysis of Napier grass, an underutilized biomass source, using ZSM-5, 0.3HZSM-5 and zinc exchanged zeolite-A catalyst. Pyrolysis was conducted in fixed bed reactor at 600 °C, 30 °C/min and 7 L/min nitrogen flow rate. The effect of catalyst-biomass ratio was evaluated with respect to pyrolysis oil yield and composition. Increasing the catalyst loading from 0.5 to 1.0 wt % showed no significant decrease in the bio-oil yield, particularly, the organic phase and thereafter decreased at catalyst loadings of 2.0 and 3.0 wt %. Standard analytical methods were used to establish the composition of the pyrolysis oil, which was made up of various aliphatic hydrocarbons, aromatics and other valuable chemicals and varied greatly with the surface acidity and pore characteristics of the individual catalysts. This study has demonstrated that pyrolysis oil with high fuel quality and value added chemicals can be produced from pyrolysis of Napier grass over acidic zeolite based catalysts.

  14. Room-temperature heterogeneous hydroxylation of phenol with hydrogen peroxide over Fe2+, Co2+ ion-exchanged Na beta zeolite.

    Science.gov (United States)

    Wang, Jun; Park, Jung-Nam; Wei, Xian-Yong; Lee, Chul Wee

    2003-03-07

    Ion-exchanged Na beta zeolite with Fe2+ and Co2+ cations shows high catalytic activity at room temperature in phenol hydroxylation with H2O2, where the conversion of phenol is ca. 21% and the selectivity of benzoquinone is below 3% at a molar ratio of phenol to H2O2 of 3 in the starting aqueous reaction medium.

  15. Superior performance of metal-organic frameworks over zeolites as solid acid catalysts in the Prins reaction: green synthesis of nopol.

    Science.gov (United States)

    Opanasenko, Maksym; Dhakshinamoorthy, Amarajothi; Hwang, Young Kyu; Chang, Jong-San; Garcia, Hermenegildo; Čejka, Jiří

    2013-05-01

    The catalytic performance of a set of metal-organic frameworks [CuBTC, FeBTC, MIL-100(Fe), MIL-100(Cr), ZIF-8, MIL-53(Al)] was investigated in the Prins condensation of β-pinene with formaldehyde and compared with the catalytic behavior of conventional aluminosilicate zeolites BEA and FAU and titanosilicate zeolite MFI (TS-1). The activity of the investigated metal-organic frameworks (MOFs) increased with the increasing concentration of accessible Lewis acid sites in the order ZIF-8zeolites BEA and FAU, which showed significantly lower selectivity to the target nopol than the MOFs. Its high activity, the preservation of its structure and active sites, and the possibility to use it in at least three catalytic cycles without loss of activity make MIL-100 (Fe) the best performing catalyst of the series for the Prins condensation of β-pinene and paraformaldehyde. Our report exemplifies the advantages of MOFs over zeolites as solid catalysts in liquid-phase reactions for the production of fine chemicals.

  16. Chromium removal by zeolite-rich materials obtained from an exhausted FCC catalyst: Influence of chromium incorporation on the sorbent structure.

    Science.gov (United States)

    Gonzalez, Maximiliano R; Pereyra, Andrea M; Torres Sánchez, Rosa M; Basaldella, Elena I

    2013-10-15

    A spent FCC catalyst was converted into a zeolitic mixture, and the product obtained was afterward used as trapping material for Cr(III) species frequently found in aqueous solutions. Eventual changes in the sorbent structure produced by Cr incorporation were studied by different characterization techniques such as point of zero charge determinations (PZC), X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDX), and infrared absorption (FTIR). The XRD and FTIR analyses indicated that chromium incorporation produces an amorphization of the material, and PZC measurements show no surface adsorption of charged chromium species. SEM and EDX analyses clearly show that after chromium sorption, the initial microspheroidal catalyst morphology was maintained, and the presence of chromium species was mainly detected in the outer microsphere surface, where the zeolite crystals were hydrothermally grown.

  17. Mechanistic studies of the methanol-to-olefin process on acidic zeolite catalysts by in situ solid-state NMR-UV/Vis spectroscopy

    OpenAIRE

    Jiang, Yijiao

    2007-01-01

    Due to the increasing demand for light olefins, the catalytic conversion of methanol-to-olefins (MTO) on acidic zeolite catalysts continues to be an industrially interesting process in heterogeneous catalysis. During the last decades, increasing efforts were made to clarify the mechanism of the MTO process. Recent progress revealed that, in the MTO process, the conversion of an equilibrium mixture of methanol and dimethyl ether (DME) is dominated by a “hydrocarbon pool” route in which methano...

  18. Studies of the Effects of Alkali Metal Oxides Promoter on the Oxidative Methylation of Toluene with Methane over KY Zeolite Catalysts

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    The toluene conversion, the selectivity to styrene and ethylbenzene( C8 selectivity) in the oxidative methylation of toluene with methane have been studied comparatively for the KY zeolite catalyst promoted with Li2O, Na2O, K2O, and Cs2O respectively. It was found that the effect of promoter decreased in the order: Cs2O>Na2O>Li2O>K2O.

  19. Synthesis and Characterization of Nano Beta Zeolite and Its Catalytic Performance for Alkylation of Benzene with Propylene%纳米Beta沸石的合成与表征及催化苯和丙烯烷基化性能

    Institute of Scientific and Technical Information of China (English)

    宗弘元; 高焕新; 魏一伦

    2015-01-01

    possessed higher concentration of total acid sites and Bronsted acid sites. As catalyst for alkylation of benzene with propylene, nano-Beta zeolite was more stable and more selective. Under the conditions of benzene to propylene molar ratio of 3.0 and reaction temperature of 150-160℃, nano-Beta zeolite exhibited the best catalytic performance. Cumene selectivity reached as high as 89% and impurity, especially,n-propylbenzene decreased to very low level. During long term industrial test, nano-Beta catalyst also had much longer life span and higher selectivity than conventional Beta.

  20. Selective catalytic reduction of NO by ammonia using mesoporous Fe-containing HZSM-5 and HZSM-12 zeolite catalysts: An option for automotive applications

    DEFF Research Database (Denmark)

    Kustov, Arkadii; Hansen, T. W.; Kustova, Marina;

    2007-01-01

    Mesoporous and conventional Fe-containing ZSM-5 and ZSM-12 catalysts (0.5–8 wt% Fe) were prepared using a simple impregnation method and tested in the selective catalytic reduction (SCR) of NO with NH3. It was found that for both Fe/HZSM-5 and Fe/HZSM-12 catalysts with similar Fe contents......, the activity of the mesoporous samples in NO SCR with NH3 is significantly higher than for conventional samples. Such a difference in the activity is probably related with the better diffusion of reactants and products in the mesopores and better dispersion of the iron particles in the mesoporous zeolite...

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

    Directory of Open Access Journals (Sweden)

    Toshiaki Hanaoka

    2015-02-01

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

  2. Application of nuclear magnetic resonance spectroscopy, Fourier transform infrared spectroscopy, UV-Visible spectroscopy and kinetic modeling for elucidation of adsorption chemistry in uptake of tetracycline by zeolite beta.

    Science.gov (United States)

    Kang, Jin; Liu, Huijuan; Zheng, Yu-Ming; Qu, Jiuhui; Chen, J Paul

    2011-02-01

    Extensive usage of tetracycline has resulted in its contamination in surface water and groundwater. The adsorption of tetracycline on zeolite beta was systematically investigated for the decontamination of the antibiotic polluted water in this study. Ninety percent of uptake by the zeolite beta occured in 0.25h, and the adsorption equilibrium was obtained within 3h, which was well described by an intraparticle diffusion model. The adsorption generally increased when pH was increased from 4.0 to 5.0, and then decreased significantly as the pH was further increased, which was caused by the pH-dependent speciation of tetracycline and surface charge of zeolite beta. Both Freundlich and Langmuir equations well described the adsorption isotherm. A thermodynamic analysis showed that the sorption process was spontaneous and endothermic. Aluminum atoms in the zeolite played a crucial role in the uptake; the adsorption increased with the increasing aluminum content in zeolite. The UV-Visible spectroscopy study showed that the spectra of tetracycline changed upon the interaction with zeolite beta, which could be ascribed to the formation of complexes of tetracycline and aluminum atoms in the zeolite surface. Nuclear magnetic resonance spectroscopy study further confirmed the participation of Al in the tetracycline adsorption. Fourier transform infrared spectroscopy studies showed that the amino functional groups in tetracycline were involved in the complexation with the zeolite surface.

  3. Evidence for an initiation of the methanol-to-olefin process by reactive surface methoxy groups on acidic zeolite catalysts.

    Science.gov (United States)

    Wang, Wei; Buchholz, Andreas; Seiler, Michael; Hunger, Michael

    2003-12-10

    Recent progress reveals that, in the methanol-to-olefin (MTO) process on acidic zeolites, the conversion of an equilibrium mixture of methanol and DME is dominated by a "hydrocarbon pool" mechanism. However, the initial C-C bond formation, that is, the chemistry during the kinetic "induction period" leading to the reactive hydrocarbon pool, still remains unclear. With the application of a stopped-flow protocol, in the present work, pure surface methoxy groups [SiO(CH(3))Al] were prepared on various acidic zeolite catalysts (H-Y, H-ZSM-5, H-SAPO-34) at temperatures lower than 473 K, and the further reaction of these methoxy species was investigated by in situ (13)C MAS NMR spectroscopy. By using toluene and cyclohexane as probe molecules which are possibly involved in the MTO process, we show the high reactivity of surface methoxy species. Most importantly, the formation of hydrocarbons from pure methoxy species alone is demonstrated for the first time. It was found that (i) surface methoxy species react at room temperature with water to methanol, indicating the occurrence of a chemical equilibrium between these species at low temperatures. In the presence of aromatics and alkanes, (ii) the reactivity of surface methoxy groups allows a methylation of these organic compounds at reaction temperatures of ca. 433 and 493 K, respectively. In the absence of water and other organic species, that is, under flow conditions and on partially methylated catalysts, (iii) a conversion of pure methoxy groups alone to hydrocarbons was observed at temperatures of T >/= 523 K. This finding indicates a possible formation of the first hydrocarbons during the kinetic induction period of the MTO process via the conversion of pure surface methoxy species (case iii). After the first hydrocarbons are formed, or in the presence of a small amount of organic impurities, surface methoxy groups contribute to a further methylation of these organic compounds (case ii), leading to the formation of

  4. Effects of Calcination Temperature on the Acidity and Catalytic Performances of HZSM-5 Zeolite Catalysts for the Catalytic Cracking of n-Butane

    Institute of Scientific and Technical Information of China (English)

    Jiangyin Lu; Zhen Zhao; Chunming Xu; Aijun Duan; Pu Zhang

    2005-01-01

    The acidic modulations of a series of HZSM-5 catalysts were successfully made by calcination at different treatment temperatures, i.e. 500, 600, 650, 700 and 800 ℃, respectively. The results indicated that the total acid amounts, their density and the amount of B-type acid of HZSM-5 catalysts rapidly decreased, while the amounts of L-type acid had almost no change and thus the ratio of L/B was obviously enhanced with the increase of calcination temperature (excluding 800 ℃). The catalytic performances of modified HZSM-5 catalysts for the cracking of n-butane were also investigated. The main properties of these catalysts were characterized by means of XRD, N2 adsorption at low temperature, NH3-TPD, FTIR of pyridine adsorption and BET surface area measurements. The results showed that HZSM-5 zeolite pretreated at 800 ℃ had very low catalytic activity for n-butane cracking. In the calcination temperature range of 500-700 ℃, the total selectivity to olefins, propylene and butene were increased with the increase of calcination temperature, while, the selectivity for arene decreased with the calcination temperature.The HZSM-5 zeolite calcined at 700 ℃ produced light olefins with high yield, at the reaction temperature of 650 ℃ the yields of total olefins and ethylene were 52.8% and 29.4%, respectively. Besides, the more important role is that high calcination temperature treatment improved the duration stability of HZSM-5zeolites. The effect of calcination temperature on the physico-chemical properties and catalytic performance of HZSM-5 for cracking of n-butane was explored. It was found that the calcination temperature had large effects on the surface area, crystallinity and acid properties of HZSM-5 catalyst, which further affected the catalytic performance for n-butane cracking.

  5. Immobilization of L-Lysine on Zeolite 4A as an Organic-Inorganic Composite Basic Catalyst for Synthesis of α,β-Unsaturated Carbonyl Compounds under Mild Conditions

    Energy Technology Data Exchange (ETDEWEB)

    Zamani, Farzad; Rezapour, Mehdi; Kianpour, Sahar [Islamic Azad Univ., Isfahan (Iran, Islamic Republic of)

    2013-08-15

    Lysine (Lys) immobilized on zeolite 4A was prepared by a simple adsorption method. The physical and chemical properties of Lys/zeolite 4A were investigated by X-ray diffraction (XRD), FT-IR, Brunauer-Emmett-Teller (BET), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and UV-vis. The obtained organic-inorganic composite was effectively employed as a heterogeneous basic catalyst for synthesis of α,β-unsaturated carbonyl compounds. No by-product formation, high yields, short reaction times, mild reaction conditions, operational simplicity with reusability of the catalyst are the salient features of the present catalyst.

  6. BTX production by in-situ contact reforming of low-temperature tar from coal with zeolite-derived catalysts; Zeolite kei shokubai wo mochiita sekitan teion tar no sesshoku kaishitsu ni yoru BTX no seisei

    Energy Technology Data Exchange (ETDEWEB)

    Matsunaga, T.; Fuda, K.; Murakami, K.; Kyo, M.; Hosoya, S.; Kobayashi, S. [Akita University, Akita (Japan). Mining College

    1996-10-28

    On BTX production process from low-temperature tar obtained by pyrolysis of coal, the effect of exchanged metallic species and reaction temperature were studied using metallic ion-exchanged Y-zeolite as catalyst. In experiment, three kinds of coals with different produced tar structures such as Taiheiyo and PSOC-830 sub-bituminous coals and Loy Yang brown coal were used. Y-zeolite ion-exchanged with metal chloride aqueous solution was used as catalyst. Zn{sup 2+}, Ni{sup 2+} and In{sup 3+} were used as metal ions to be exchanged. The experiment was conducted by heating a pyrolysis section up to 600{degree}C for one hour after preheating a contact reforming section up to a certain proper temperature. As a result, the Ni system catalyst was effective for BTX production from aromatic-abundant tar, while the Zn system one from lower aromatic tar. In general, relatively high yields of toluene and xylene were obtained at lower temperature, while those of benzene at higher temperature. 4 figs., 1 tab.

  7. Light straight-run gas oil hydrotreatment over sulfided CoMoP/Al{sub 2}O{sub 3}-USY zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Marin, C.; Escobar, J.; Galvan, E.; Murrieta, F.; Zarate, R.; Vaca, H. [Instituto Mexicano del Petroleo, Tratamiento de Crudo Maya, Eje Central Lazaro Cardenas 152, Col. San Bartolo Atepehuacan, Del. G.A. Madero (Mexico)

    2005-01-25

    Al{sub 2}O{sub 3} supports were modified by integrating USY zeolites (13.6 wt.%) of various nominal SiO{sub 2}/Al{sub 2}O{sub 3} molar ratios (30-80). The obtained hybrid solids calcined at 500 {sup o}C were impregnated at incipient wetness with a Co-Mo-P solution. After sulfiding with CS{sub 2}-spiked naphtha (at 230 {sup o}C, 5.5 MPa and LHSV=3 h{sup -1}) the corresponding catalysts were tested in light straight-run gas oil hydrotreatment at industrially relevant operating conditions. The catalyst containing zeolite of the highest SiO{sub 2}/Al{sub 2}O{sub 3} molar ratio (80) showed very high hydrodesulfurization activity. Operating at 360 {sup o}C, 5.5 MPa and LHSV=2.5 h{sup -1}, ultra-low sulfur diesel (circa 50 ppm S) could be obtained over that material, from a feedstock of 10,400 ppm S. Medium-strong acidity could be playing an important role on this behaviour by promoting isomerization of sterically hindered organo-sulfur compounds to more favorable configurations. Moreover, hydrodearomatization and hydrodenitrogenation were also enhanced by addition of that high-silica zeolite.

  8. Sn-Beta zeolites with borate salts catalyse the epimerization of carbohydrates via an intramolecular carbon shift.

    Science.gov (United States)

    Gunther, William R; Wang, Yuran; Ji, Yuewei; Michaelis, Vladimir K; Hunt, Sean T; Griffin, Robert G; Román-Leshkov, Yuriy

    2012-01-01

    Carbohydrate epimerization is an essential technology for the widespread production of rare sugars. In contrast to other enzymes, most epimerases are only active on sugars substituted with phosphate or nucleotide groups, thus drastically restricting their use. Here we show that Sn-Beta zeolite in the presence of sodium tetraborate catalyses the selective epimerization of aldoses in aqueous media. Specifically, a 5 wt% aldose (for example, glucose, xylose or arabinose) solution with a 4:1 aldose:sodium tetraborate molar ratio reacted with catalytic amounts of Sn-Beta yields near-equilibrium epimerization product distributions. The reaction proceeds by way of a 1,2 carbon shift wherein the bond between C-2 and C-3 is cleaved and a new bond between C-1 and C-3 is formed, with C-1 moving to the C-2 position with an inverted configuration. This work provides a general method of performing carbohydrate epimerizations that surmounts the main disadvantages of current enzymatic and inorganic processes.

  9. Zeolites and Usage Areas

    Directory of Open Access Journals (Sweden)

    Jale Gülen

    2012-06-01

    Full Text Available Zeolites are formed via several reactions from the minerals that consist of aluminium and silica. Zeolites, which have a growing significance in recent days are one of important industrial raw materials. As well as being used as a catalyst, theirability to do ion exchange and adsorption make them even more valuable. Zeolites are used in several industries such as energy, agriculture and animal husbandry, mining and metallurgy, construction, detergent, paper, etc. In this study, the definiton, formation and usage areas of zeolites are explained.

  10. Selective catalytic reduction of nitrogen oxides with ammonia over microporous zeolite catalysts

    OpenAIRE

    VENNESTROM, PETER NICOLAI RAVNBORG

    2014-01-01

    With increasing legislative demands to remove nitrogen oxides (NOx) from automotive diesel exhaust, new catalyst systems are investigated and intensely studied in industry as well in academia. The most prevailing catalytic method of choice is the selective catalytic reduction (SCR) where non-toxic urea is used as a reductant for practical reasons. Usually urea is stored in a separate tank and once injected into the exhaust system it hydrolyses into the more aggressive reductant NH3 and CO2. ...

  11. A Comparative Study of N2O Formation during the Selective Catalytic Reduction of NOx with NH3 on Zeolite Supported Cu Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Hai-Ying; Wei, Zhehao; Kollar, Marton; Gao, Feng; Wang, Yilin; Szanyi, Janos; Peden, Charles HF

    2015-09-01

    A comparative study was carried out on a small-pore CHA.Cu and a large-pore BEA.Cu zeolite catalyst to understand the lower N2O formation on small-pore zeolite supported Cu catalysts in the selective catalytic reduction (SCR) of NOx with NH3. On both catalysts, the N2O yield increases with an increase in the NO2/NOx ratios of the feed gas, suggesting N2O formation via the decomposition of NH4NO3. Temperature-programmed desorption experiments reveal that NH4NO3 is more stable on CHA.Cu than on BEA.Cu. In situ FTIR spectra following stepwise (NO2 + O2) and (15NO + NH3 + O2) adsorption and reaction, and product distribution analysis using isotope-labelled reactants, unambiguously prove that surface nitrate groups are essential for the formation of NH4NO3. Furthermore, CHA.Cu is shown to be considerably less active than BEA.Cu in catalyzing NO oxidation and the subsequent formation of surface nitrate groups. Both factors, i.e., (1) the higher thermal stability of NH4NO3 on CHA.Cu, and (2) the lower activity for this catalyst to catalyze NO oxidation and the subsequent formation of surface nitrates, likely contribute to the higher SCR selectivity with less N2O formation on this catalyst as compared to BEA.Cu. The latter is determined as the primary reason since surface nitrates are the source that leads to the formation of NH4NO3 on the catalysts.

  12. NO oxidation on Zeolite Supported Cu Catalysts: Formation and Reactivity of Surface Nitrates

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Hai-Ying; Wei, Zhehao; Kollar, Marton; Gao, Feng; Wang, Yilin; Szanyi, Janos; Peden, Charles HF

    2016-04-18

    The comparative activities of a small-pore Cu-CHA and a large-pore Cu-BEA catalyst for the selective catalytic reduction (SCR) of NOx with NH3, and for the oxidation of NO to NO2 and the subsequent formation of surface nitrates were investigated. Although both catalysts are highly active in SCR reactions, they exhibit very low NO oxidation activity. Furthermore, Cu-CHA is even less active than Cu-BEA in catalyzing NO oxidation but is clearly more active for SCR reactions. Temperature-programed desorption (TPD) experiments following the adsorption of (NO2 + NO + O2) with different NO2:NO ratios reveal that the poor NO oxidation activity of the two catalysts is not due to the formation of stable surface nitrates. On the contrary, NO is found to reduce and decompose the surface nitrates on both catalysts. To monitor the reaction pathways, isotope exchange experiments were conducted by using 15NO to react with 14N-nitrate covered catalyst surfaces. The evolution of FTIR spectra during the isotope exchange process demonstrates that 14N-nitrates are simply displaced with no formation of 15N-nitrates on the Cu-CHA sample, which is clearly different from that observed on the Cu-BEA sample where formation of 15N-nitrates is apparent. The results suggest that the formal oxidation state of N during the NO oxidation on Cu-CHA mainly proceeds from its original +2 to a +3 oxidation state, whereas reaching a higher oxidation state for N, such as +4 or +5, is possible on Cu-BEA. The authors at PNNL gratefully acknowledge the US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Vehicle Technologies Office for the support of this work. The research described in this paper was performed at the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the US DOE by Battelle.

  13. Template-synthesized porous silicon carbide as an effective host for zeolite catalysts.

    Science.gov (United States)

    Gu, Lijun; Ma, Ding; Yao, Songdong; Liu, Xiumei; Han, Xiuwen; Shen, Wenjie; Bao, Xinhe

    2009-12-14

    A facile method has been developed for the fabrication of porous silicon carbide (SiC) by means of sintering a mixture of SiC powder and carbon pellets at a relatively lower temperature, that is, 1450 degrees C, in air. The pore density and the total pore volume of the resulting porous SiC could be tuned by changing the initial SiC/C weight ratio. The structure evolution and the associated property changes during the preparation were examined through X-ray diffraction, scanning electron microscopy, thermogravimetric analysis, (29)Si magic-angle spinning (MAS) NMR spectroscopy, and mercury-intrusion porosimetry analyses. Silica and SiO(x)C(y) ceramics formed in situ during the calcination process acted as binders of the porous SiC grains. The porous SiC can be used as a host for the growth of ZSM-5 zeolite crystals to form the ZSM-5/porous-SiC composite material. After loading another catalytic active component of molybdenum, a novel catalytic material, Mo-ZSM-5/porous-SiC, was obtained, which exhibited improved catalytic activity in the methane dehydroaromatization reaction.

  14. H-ZSM-5 Zeolite Synthesis by Sourcing Silica from the Wheat Husk Ash: Characterization and Application as a Versatile Heterogeneous Catalyst in Organic Transformations including Some Multicomponent Reactions

    Directory of Open Access Journals (Sweden)

    Isak Rajjak Shaikh

    2015-01-01

    Full Text Available ZSM-5 zeolite was synthesized by sourcing silica from wheat husk ash and was converted into its protonated form following careful, conventionally accepted ion-exchange method and calcinations. The H-ZSM-5 zeolite (Si/Al ratio = 30 prepared was appropriately characterized by XRD, FT-IR, SEM, TEM, TG-DTA, CV, and so forth, and evaluated as recyclable catalyst in selective organic transformations including three- and four-component reactions. The catalytic activity of the zeolite sample supposedly relates to increased density of the accessible acid sites.

  15. Lanthanum-catalysed synthesis of microporous 3D graphene-like carbons in a zeolite template

    Science.gov (United States)

    Kim, Kyoungsoo; Lee, Taekyoung; Kwon, Yonghyun; Seo, Yongbeom; Song, Jongchan; Park, Jung Ki; Lee, Hyunsoo; Park, Jeong Young; Ihee, Hyotcherl; Cho, Sung June; Ryoo, Ryong

    2016-07-01

    Three-dimensional graphene architectures with periodic nanopores—reminiscent of zeolite frameworks—are of topical interest because of the possibility of combining the characteristics of graphene with a three-dimensional porous structure. Lately, the synthesis of such carbons has been approached by using zeolites as templates and small hydrocarbon molecules that can enter the narrow pore apertures. However, pyrolytic carbonization of the hydrocarbons (a necessary step in generating pure carbon) requires high temperatures and results in non-selective carbon deposition outside the pores. Here, we demonstrate that lanthanum ions embedded in zeolite pores can lower the temperature required for the carbonization of ethylene or acetylene. In this way, a graphene-like carbon structure can be selectively formed inside the zeolite template, without carbon being deposited at the external surfaces. X-ray diffraction data from zeolite single crystals after carbonization indicate that electron densities corresponding to carbon atoms are generated along the walls of the zeolite pores. After the zeolite template is removed, the carbon framework exhibits an electrical conductivity that is two orders of magnitude higher than that of amorphous mesoporous carbon. Lanthanum catalysis allows a carbon framework to form in zeolite pores with diameters of less than 1 nanometre; as such, microporous carbon nanostructures can be reproduced with various topologies corresponding to different zeolite pore sizes and shapes. We demonstrate carbon synthesis for large-pore zeolites (FAU, EMT and beta), a one-dimensional medium-pore zeolite (LTL), and even small-pore zeolites (MFI and LTA). The catalytic effect is a common feature of lanthanum, yttrium and calcium, which are all carbide-forming metal elements. We also show that the synthesis can be readily scaled up, which will be important for practical applications such as the production of lithium-ion batteries and zeolite-like catalyst

  16. Session 6: Decomposition of NO over {beta}-Mo{sub 2}C and {beta}-Mo{sub 2}C/Al{sub 2}O{sub 3} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Shengfu, Ji; Chengyue, Li [Beijing University of Chemical Technology, Key Lab. of Science and Technology of Controllable Chemical Reactions, Ministry of Education (China); Shengfu, Ji; Jiaxin, Wang; Jian, Yang; Shuben, Li [State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou (China)

    2004-07-01

    In this study, for the first time it has been found that the the bulk {beta}-Mo{sub 2}C and an alumina-supported {beta}-Mo{sub 2}C catalysts are very active for the direct NO decomposition at low temperature. The obtained experimental results are presented. (authors)

  17. Enhancement of Treatment Efficiency of Recalcitrant Wastewater Containing Textile Dyes Using a Newly Developed Iron Zeolite Socony Mobil-5 Heterogeneous Catalyst.

    Science.gov (United States)

    Ahmad, Mushtaq; Asghar, Anam; Abdul Raman, Abdul Aziz; Wan Daud, Wan Mohd Ashri

    2015-01-01

    Fenton oxidation, an advanced oxidation process, is an efficient method for the treatment of recalcitrant wastewaters. Unfortunately, it utilizes H2O2 and iron-based homogeneous catalysts, which lead to the formation of high volumes of sludge and secondary pollutants. To overcome these problems, an alternate option is the usage of heterogeneous catalyst. In this study, a heterogeneous catalyst was developed to provide an alternative solution for homogeneous Fenton oxidation. Iron Zeolite Socony Mobile-5 (Fe-ZSM-5) was synthesized using a new two-step process. Next, the catalyst was characterized by scanning electron microscopy, energy-dispersive X-ray spectroscopy, fourier transform infrared spectroscopy, and Brunauer-Emmett-Teller analysis and tested against a model wastewater containing the azo dye Acid Blue 113. Results showed that the loading of iron particles reduced the surface area of the catalyst from 293.59 to 243.93 m2/g; meanwhile, the average particle size of the loaded material was 12.29 nm. Furthermore, efficiency of the developed catalyst was evaluated by performing heterogeneous Fenton oxidation. Taguchi method was coupled with principal component analysis in order to assess and optimize mineralization efficiency. Experimental results showed that under optimized conditions, over 99.7% degradation and 77% mineralization was obtained, with a 90% reduction in the consumption of the developed catalyst. Furthermore, the developed catalyst was stable and reusable, with less than 2% leaching observed under optimized conditions. Thus, the present study proved that newly developed catalyst has enhanced the oxidation process and reduced the chemicals consumption.

  18. Application of aromatization catalyst in synthesis of carbon nanotubes

    Indian Academy of Sciences (India)

    Song Rongjun; Yang Yunpeng; Ji Qing; Li Bin

    2012-02-01

    In a typical chemical vapour deposition (CVD) process for synthesizing carbon nanotubes (CNTs), it was found that the aromatization catalysts could promote effectively the formation of CNT. The essence of this phenomenon was attributed to the fact that the aromatization catalyst can accelerate the dehydrogenation–cyclization and condensation reaction of carbon source, which belongs to a necessary step in the formation of CNTs. In this work, aromatization catalysts, H-beta zeolite, HZSM-5 zeolite and organically modified montmorillonite (OMMT) were chosen to investigate their effects on the formation of multi-walled carbon nanotubes (MWCNTs) via pyrolysis method when polypropylene and 1-hexene as carbon source and Ni2O3 as the charring catalyst. The results demonstrated that the combination of those aromatization catalysts with nickel catalyst can effectively improve the formation of MWCNTs.

  19. I. Synthesis, characterization, and base catalysis of novel zeolite supported super-basic materials II. Oxidative dehydrogenation of ethane over reduced heteropolyanion catalysts

    Science.gov (United States)

    Galownia, Jonathan M.

    reliable precursor for the formation of zeolite supported super-basic materials. The second part of this thesis describes the oxidative dehydrogenation of ethane over partially reduced heteropolyanions. Niobium and pyridine exchanged salts of phosphomolybdic (NbPMo12Pyr) and phosphovanadomolybdic (NbPMo11VPyr) acids are investigated as catalyst precursors to prepare materials for catalyzing the oxidative dehydrogenation of ethane to ethylene and acetic acid at atmospheric pressure. The effects of feed composition, steam flow, temperature, and precursor composition on catalytic activity and selectivity are presented for both ethane and ethylene oxidation. Production of ethylene and acetic acid from ethane using the catalytic materials exceeds that reported in the literature for Mo-V-Nb-Ox systems under atmospheric or elevated pressure. Production of acetic acid from ethylene is also greater than that observed for Mo-V-Nb-Ox systems. Addition of vanadium reduces catalytic activity and selectivity to both ethylene and acetic acid while niobium is essential for the formation of acetic acid from ethane. Other metals such as antimony, iron, and gallium do not provide the same beneficial effect as niobium. Molybdenum in close proximity to niobium is the active site for ethane activation while niobium is directly involved in the transformation of ethylene to acetic acid. A balance of niobium and protonated pyridine is required to produce an active catalyst. Water is found to aid in desorption of acetic acid, thereby limiting deep oxidation to carbon oxides. A reaction scheme is proposed for the production of acetic acid from ethane over the catalytic materials.

  20. Dimethyl ether synthesis via methanol and syngas over rare earth metals modified zeolite Y and dual Cu-Mn-Zn catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Dingfeng Jin; Bing Zhu; Zhaoyin Hou; Jinhua Fei; Hui Lou; Xiaoming Zheng [Zhejiang University, Hangzhou (China). Institute of Catalysis, Department of Chemistry

    2007-12-15

    A series of zeolite Y modified with La, Ce, Pr, Nd, Sm and Eu were prepared via ion-exchange, and characterized by XRD, FT-IR and NH{sub 3}-TPD. It was found that these rare earth metals were encapsulated in the supercage of zeolite Y and resulted in its enhanced acidity. Among them, La-, Ce-, Pr- and Nd-modified zeolite Y exhibited higher activity and stability (than pure HY) for methanol dehydration to dimethyl ether (DME). For DME synthesis directly from CO hydrogenation using the dual Cu-Mn-Zn/modified-Y catalysts, it was found that Cu-Mn-Zn/La-Y and Cu-Mn-Zn/Ce-Y were more active than Cu-Mn-Zn/pure-HY. The conversion of CO on Cu-Mn-Zn/Ce-HY achieved 77.1% in an isothermal fixed bed reactor at 245{sup o}C, 2.0 MPa, H{sub 2}/CO = 3/2 and 1500 h{sup -1}. 36 refs., 7 figs., 3 tabs.

  1. An investigation of the activity and stability of Pd and Pd-Zr modified Y-zeolite catalysts for the removal of PAH, CO, CH{sup 4} and NO{sup x} emissions

    Energy Technology Data Exchange (ETDEWEB)

    Klingstedt, F.; Kalantar Neyestanaki, A.; Lindfors, L.-E.; Salmi, T. [Process Chemistry Group, Laboratory of Industrial Chemistry, Abo Akademi University, Biskopsg. 8, FIN-20500 Turku (Finland); Heikkila, T.; Laine, E. [Laboratory of Industrial Physics, Department of Physics, University of Turku, Vesilinnant. 5, FIN-20014 Turku (Finland)

    2003-01-30

    Pd-Y- and Pd-Zr-Y-zeolite catalysts were prepared by the ion-exchange of parent NH{sub 3}-Y-zeolite, thermally pre-treated Y-zeolite and hydrothermally pre-treated Y-zeolite. The activity of the catalysts was studied in conversion of gas mixtures simulating the flue gases from the combustion of biofuels and natural gas driven vehicles (NGVs) at temperature ranges of 120-800C. The effect of sulphur-poisoning was examined by the addition of 5ppm SO{sub 2} into the feed gas mixtures. High activity in the removal of the model pollutants was obtained over the fresh catalysts. De-activation was observed as a result of catalyst ageing in the reactants' flow (800C, 6h) or steam treatment (850C, 12vol.% H{sub 2}O, 16h). The de-activation was attributed to the de-alumination as well as to the migration of Pd{sup 2+} cations. The catalysts were characterised by XRD, SEM-EDXA, N{sub 2}-physisorption, O{sub 2}/SO{sub 2}/NH{sub 3}/naphthalene-TPD, XRF and DCP.

  2. Mo-Based Zeolite Catalysts and Oxygen-Free Methane Aromatization%Mo基分子筛催化剂及甲烷无氧芳构化

    Institute of Scientific and Technical Information of China (English)

    胥月兵; 陆江银; 王吉德; 张战国

    2011-01-01

    Among the investigated catalysts, the Mo-based zeolite catalysts showed the highest catalytic activity. These catalysts were systematically discussed on MoOx structure and its location in zeolite, the active Mo species and its carburization in the induction period. The issues on intermediates, the bi-functional reaction mechanism and catalyst deactivation with coke were also discussed. The effect of preparation method, calcination temperature and time, Mo loading, ratio of SiO2 to Al2O3 and the catalyst pretreatment in reaction on the catalytic performance of Mo-based catalyst were demonstrated. Then the ways to improve the catalyst activity and reaction stability were comprehensively introduced, pointing out that the catalyst was always deactivated due to coke and needed regeneration. At last according to our research results the discussion and analysis in the view of engineering technology for methane dehydroaromatization were given, and some problems needed to be solved were put forward.%本文综述了甲烷无氧芳构化反应及Mo基分子筛催化剂的研究进展.在众多的催化剂中以Mo基分子筛催化性能最佳.概括了催化剂中关于MoOz前躯体结构和其在分子筛中落位,Mo2C物种和诱导期等;讨论了反应中涉及的中间产物、双功能机理以及催化剂失活等问题;归纳了催化剂制备过程中制备方法、焙烧温度与时间、Mo载量和分子筛硅铝比以及催化剂预处理对反应活性的影响;综述了提高催化剂催化性能和反应性能的各种方法,并对其分析,同时介绍了两种催化剂再生方法.最后,依据本实验室研究进展,对甲烷芳构化从工艺角度进行一些可行性讨论,并提出相关问题和展望.

  3. Catalytic Combustion of Ethyl Acetate over Nanostructure Cobalt Supported ZSM-5 Zeolite Catalysts

    Institute of Scientific and Technical Information of China (English)

    NIAEI,Aligholi; SALARI,Dariush; HOSSEINI,Seyed Ali; KHATAMIAN,Masumeh; JODAEL,Azadeh

    2009-01-01

    Gas phase catalytic combustion of ethyl acetate,as one of volatile organic compounds(VOC),was studied on nanostructure ZSM-5.HZSM-5 and Co-ZSM-5 with different cobalt loadings. Nanostructure of ZSM-5 Was deter-mined by XRD,SEM and TEM. Catalytic studies were carried out under atmospheric pressure in a fixed bed reactor.Results showed that the Co-ZSM-5 catalysts had better activity than others and at temperatures below 350℃.amount of Co loading was mole effective on catalytic activity.The order of conversion of ethyl acetate over differ-ent Co loading is as follows:Co-ZSM-5(0.75 wt%)

  4. Potential of sustainable hierarchical zeolites in the valorization of α-pinene.

    Science.gov (United States)

    Nuttens, Nicolas; Verboekend, Danny; Deneyer, Aron; Van Aelst, Joost; Sels, Bert F

    2015-04-13

    In the valorization of α-pinene, which is an important biomass intermediate derived from turpentine oil, hierarchical (mesoporous) zeolites represent a superior class of catalysts. Hierarchical USY, ZSM-5, and beta zeolites have been prepared, characterized, and catalytically evaluated, with the aim of combining the highest catalytic performance with the most sustainable synthetic protocol. These zeolites are prepared by alkaline treatment in aqueous solutions of NH4 OH, NaOH, diethylamine, and NaOH complemented with tetrapropylammonium bromide. The hierarchical USY zeolite is the most attractive catalyst of the tested series, and is able to combine an overall organic-free synthesis with an up to sixfold activity enhancement and comparable selectivity over the conventional USY zeolite. This superior performance relates to a threefold greater activity than that of the commercial standard, namely, H2 SO4 /TiO2 . Correlation of the obtained benefits to the amount of solid lost during the postsynthetic modifications highlights that the highest activity gains are obtained with minor leaching. Furthermore, a highly zeolitic character, as determined by bulk XRD, is beneficial, but not crucial, in the conversion of α-pinene. The alkaline treatments not only result in a higher overall activity, but also a more functional external surface area, attaining up to four times the pinene conversions per square nanometer. The efficiency of the hierarchical USY zeolite is concomitantly demonstrated in the conversion of limonene and turpentine oil, which emphasizes its industrial potential.

  5. SSZ-52, a zeolite with an 18-layer aluminosilicate framework structure related to that of the DeNOx catalyst Cu-SSZ-13.

    Science.gov (United States)

    Xie, Dan; McCusker, Lynne B; Baerlocher, Christian; Zones, Stacey I; Wan, Wei; Zou, Xiaodong

    2013-07-17

    A new zeolite (SSZ-52, |(C14H28N)6Na6(H2O)18|[Al12Si96O216]), related to the DeNOx catalyst Cu-SSZ-13 (CHA framework type), has been synthesized using an unusual polycyclic quaternary ammonium cation as the structure-directing agent. By combining X-ray powder diffraction (XPD), high-resolution transmission electron microscopy (HRTEM) and molecular modeling techniques, its porous aluminosilicate framework structure (R3m, a = 13.6373(1) Å, c = 44.7311(4) Å), which can be viewed as an 18-layer stacking sequence of hexagonally arranged (Si,Al)6O6 rings (6-rings), has been elucidated. The structure has a three-dimensional 8-ring channel system and is a member of the ABC-6 family of zeolites (those that can be described in terms of 6-ring stacking sequences) like SSZ-13, but it has cavities that are twice as large. The code SFW has been assigned to this new framework type. The large cavities contain pairs of the bulky organic cations. HRTEM and XPD simulations show that stacking faults do occur, but only at the 5-10% level. SSZ-52 has considerable potential as a catalyst in the areas of gas conversion and sequestration.

  6. Structure and nuclearity of active sites in Fe-zeolites: comparison with iron sites in enzymes and homogeneous catalysts.

    Science.gov (United States)

    Zecchina, Adriano; Rivallan, Mickaël; Berlier, Gloria; Lamberti, Carlo; Ricchiardi, Gabriele

    2007-07-21

    Fe-ZSM-5 and Fe-silicalite zeolites efficiently catalyse several oxidation reactions which find close analogues in the oxidation reactions catalyzed by homogeneous and enzymatic compounds. The iron centres are highly dispersed in the crystalline matrix and on highly diluted samples, mononuclear and dinuclear structures are expected to become predominant. The crystalline and robust character of the MFI framework has allowed to hypothesize that the catalytic sites are located in well defined crystallographic positions. For this reason these catalysts have been considered as the closest and best defined heterogeneous counterparts of heme and non heme iron complexes and of Fenton type Fe(2+) homogeneous counterparts. On this basis, an analogy with the methane monooxygenase has been advanced several times. In this review we have examined the abundant literature on the subject and summarized the most widely accepted views on the structure, nuclearity and catalytic activity of the iron species. By comparing the results obtained with the various characterization techniques, we conclude that Fe-ZSM-5 and Fe-silicalite are not the ideal samples conceived before and that many types of species are present, some active and some other silent from adsorptive and catalytic point of view. The relative concentration of these species changes with thermal treatments, preparation procedures and loading. Only at lowest loadings the catalytically active species become the dominant fraction of the iron species. On the basis of the spectroscopic titration of the active sites by using NO as a probe, we conclude that the active species on very diluted samples are isolated and highly coordinatively unsaturated Fe(2+) grafted to the crystalline matrix. Indication of the constant presence of a smaller fraction of Fe(2+) presumably located on small clusters is also obtained. The nitrosyl species formed upon dosing NO from the gas phase on activated Fe-ZSM-5 and Fe-silicalite, have been analyzed

  7. Effect of Fe Ion-Exchanged BEA Zeolite Catalysts on N{sub 2}O Decomposition Reaction Following Heat-treatment Temperatures

    Energy Technology Data Exchange (ETDEWEB)

    Jeong, Gi-Rim; Lee, Seung-Jae; Ryu, In-Soo; Moon, Seung-Hyun [Korea Institute of Energy Research, Daejeon (Korea, Republic of)

    2013-10-15

    The effect of heat-treatment temperature on the activity of catalysts was studied by investigating N{sub 2}O decomposition reaction in Fe ion-supported BEA Zeolite. As a result of N{sub 2}O decomposition reaction experiment, N{sub 2}O decomposition activity significantly decreased as heat-treatment temperature of Fe/BEA catalyst increased. the shape and size of the particles of Fe/BEA catalyst following the rise of heat-treatment temperature did not display a significant change. But following the rise of the heat-treatment temperature, its surface area was significantly reduced. Also it was confirmed that as the heat-treatment temperature rose, the crystallization of β structure was greatly reduced. And as heat-treatment temperature rose, while SiO structure either increased or did not exhibit much change, the structure of Fe bonded with lattice structure was speculated to decrease. From the stated results, it was concluded that the increase of heat-treatment temperature became the cause of the declined activity of catalysts by destruction of its β structure of bonding aluminium and Fe atoms.

  8. Conversion of syngas to liquid hydrocarbons over a two-component (Cr{sub 2}O{sub 3}-ZnO and ZSM-5 zeolite) catalyst: kinetic modelling and catalyst deactivation

    Energy Technology Data Exchange (ETDEWEB)

    Erena, J.; Arandes, J.M.; Bilbao, J.; Gayubo, A.G. [Universidad del Pais Vasco, Bilbao (Spain). Dept. de Ingeneria Quimica; De Lasa, H.I. [University of Western Ontario, London, ONT (Canada). Chemical Reactor Engineering Centre

    2000-05-01

    The present study describes the kinetics of syngas transformation into liquid hydrocarbons (boiling point in the gasoline range) using as catalyst a mixture of a metallic component, Cr{sub 2}O{sub 3}-ZnO, and of an acidic component, ZSM-5 zeolite. Experimental results were obtained in an isothermal fixed-bed integral reactor. The validity of several kinetic models, available for methanol synthesis, is analysed and modifications are proposed. These changes involve a rate equation with a CO{sub 2} concentration-dependent term. Catalyst deactivation is also evaluated and the effect of the operating conditions on coke deposition is established. Moreover, the rate of CO conversion and the change of catalytic activity with time-on-stream were described using a kinetic model showing a weak influence of temperature. (Author)

  9. Efficient isomerization of glucose to fructose over zeolites in consecutive reactions in alcohol and aqueous media.

    Science.gov (United States)

    Saravanamurugan, Shunmugavel; Paniagua, Marta; Melero, Juan A; Riisager, Anders

    2013-04-10

    Isomerization reactions of glucose were catalyzed by different types of commercial zeolites in methanol and water in two reaction steps. The most active catalyst was zeolite Y, which was found to be more active than the zeolites beta, ZSM-5, and mordenite. The novel reaction pathway involves glucose isomerization to fructose and subsequent reaction with methanol to form methyl fructoside (step 1), followed by hydrolysis to re-form fructose after water addition (step 2). NMR analysis with (13)C-labeled sugars confirmed this reaction pathway. Conversion of glucose for 1 h at 120 °C with H-USY (Si/Al = 6) gave a remarkable 55% yield of fructose after the second reaction step. A main advantage of applying alcohol media and a catalyst that combines Brønsted and Lewis acid sites is that glucose is isomerized to fructose at low temperatures, while direct conversion to industrially important chemicals like alkyl levulinates is viable at higher temperatures.

  10. Altering bio-oil composition by catalytic treatment of pinewood pyrolysis vapors over zeolites using an auger - packed bed integrated reactor system

    Directory of Open Access Journals (Sweden)

    Vamshi Krishna Guda

    2016-09-01

    Full Text Available Pine wood pyrolysis vapors were catalytically treated using Zeolite catalysts. An auger fed reactor was used for the pinewood pyrolysis while a packed bed reactor mounted on the top of the auger reactor housed the catalyst for the treatment of pinewood pyrolytic vapors. The pyrolytic vapors produced at 450 oC were passed through zeolite catalysts maintained at 425 oC at a weight hourly space velocity (WHSV of 12 h-1. Five zeolites, including ZSM-5, mordenite, ferrierite, Zeolite-Y, and Zeolite-beta (all in H form, were used to study the effect of catalyst properties such as acidity, pore size, and pore structure on catalytic cracking of pinewood pyrolysis vapors. Product bio-oils were analyzed for their chemical composition using GC-MS, water content, density, viscosity, acid value, pH, and elemental compositions. Thermogravimetric analysis (TGA was performed to analyze the extent of coking on zeolite catalysts. Application of catalysis to biomass pyrolysis increased gas product yields at the expense of bio-oil yields. While all the zeolites deoxygenated the pyrolysis vapors, ZSM-5 was found to be most effective. The ZSM-5 catalyzed bio-oil, rich in phenolics and aromatic hydrocarbons, was less viscous, had relatively lower acid number and high pH, and possessed oxygen content nearly half that of un-catalyzed bio-oil. Brønsted acidity, pore size, and shape-selective catalysis of ZSM-5 catalyst proved to be the determining factors for its activity. TGA results implied that the pore size of catalysts highly influenced coking reactions. Regeneration of the used catalysts was successfully completed at 700 oC.

  11. Molecular simulations of adsorption and diffusion of NO and NH3 over zeolite catalysts with various structure configurations%Industrial Catalysis

    Institute of Scientific and Technical Information of China (English)

    李懿; 刘宁; 张润铎; 李英霞

    2016-01-01

    基于巨正则蒙特卡洛和分子动力学,对NH3-SCR反应体系中吸附质分子( NO与NH3)在不同拓扑结构沸石分子筛( LTL、FER、LEV、BEA、MOR、FAU、CHA和MFI)上的吸附和扩散特性进行系统研究。结果表明,对于全硅分子筛而言,其分子筛的拓扑结构影响NO与NH3在分子筛上的吸附,综合吸附量及吸附作用能发现,MFI和LEV分子筛对NO具有较优的吸附特性;MFI和BEA分子筛对NH3具有较优的吸附特性。研究了Si与Al物质的量比对BEA分子筛吸附性能影响,结果表明,随着Si与Al物质的量比降低,分子筛自由体积逐渐增加,进而有助于分子筛催化剂对NO和NH3的吸附。采用分子动力学模拟计算NO与NH3在不同构型全硅分子筛上的扩散系数,发现具有三维直通道且孔径较大的分子筛催化剂有利于NO和NH3在其孔道内部的扩散,MFI虽然具备三维孔道结构,但由于存在Z型交叉通道,一定程度阻碍了反应物分子的扩散。%The adsorption and diffusion of NO and NH3 as the reactant of NH3-SCR reaction system over various kinds of zeolite catalysts( LTL,FER,LEV,BEA,MOR,FAU,CHA,MFI)were investigated by employing molecule simulation methods of Monte Carlo and Molecular Dynamics. The results indicated that the zeolitic topology greatly influenced the adsorption of NO and NH3 molecules according to the sim-ulation results of adsorption amount and adsorption energy. Accordingly,it was found that MFI and LEV were efficient for NO adsorption,and MFI and BEA were efficient for NH3 adsorption. The effects of Si/Al molar ratio on the adsorption of NO and NH3 over BEA zeolite were also studied. The study showed that the free volume of zeolite catalysts gradually increased along with the decrease of Si/Al molar ratios, which facilitated the adsorption of NO and NH3 . The molecular dynamics was further employed for the cal-culations of diffusion coefficient of NO and NH3 on all

  12. Hexane cracking over steamed phosphated zeolite H-ZSM-5 : Promotional effect on catalyst performance and stability

    NARCIS (Netherlands)

    Van Der Bij, Hendrik E.; Meirer, Florian; Kalirai, Samanbir; Wang, Jian; Weckhuysen, Bert M.

    2014-01-01

    The nature behind the promotional effect of phosphorus on the catalytic performance and hydrothermal stability of zeolite H-ZSM-5 has been studied using a combination of 27Al and 31P MAS NMR spectroscopy, soft X-ray absorption tomography and n-hexane catalytic cracking, complemented with NH3 tempera

  13. Modification of HZSM- 5 Zeolite by Hydrochloric Acid and Catalytic Performance of Mo - based Catalyst for Methane Dehydroaromatization Reaction%盐酸改性HZSM-5及Mo-基催化剂的MDA反应活性

    Institute of Scientific and Technical Information of China (English)

    王红霞; 赵婷婷

    2012-01-01

    采用盐酸溶液在303K对HZSM-5分子筛进行预处理,并以处理后的分子筛制备相应的Mo-基催化剂.分子筛和催化剂采用XRD和NH3-TPD等手段进行表征,利用甲烷无氧芳构化(MDA)反应评价Mo-基催化剂的催化活性.结果表明,指定实验条件下的盐酸处理在一定程度上降低了分子筛的结晶度,降低了分子筛上的B酸量,改性后的Mo-基催化剂在MDA反应中表现很好的稳定性.%The pretreatment with HC1 solution at 303 K was applied to modify HZSM -5 zeolite, and the Mobased catalysts were prepared by using the modified HZSM -5 zeolite as support and tested for catalytic performance of methane dehydroaromatization reaction. The modified Mo - based catalysts show a higher stability than that of Mo/HZSM - 5 catalyst prepared with unmodified with HZSM - 5 zeolite. The effect of acid treatment on the structure and acidity of HZSM - 5 zeolite and Mo - based catalysts were studied by XRD and NH3 - TPD methods. The results show that the acid treatment to HZSM - 5 at given experimental conditions led to a decrease in the crystallinity of HZSM -5 zeolite and the number of the Brnsted acid sites to a certain degree.

  14. Beta﹣USY复配对柴油加氢改质催化剂性能的影响%INFLUENCE OF COUPLED BETA AND USY ON PERFORMANCE OF HYDROUPGRADING CATALYSTS

    Institute of Scientific and Technical Information of China (English)

    刘晨光; 孟健; 张孔远; 韩冰

    2014-01-01

    A series of Ni﹣W∕Beta﹣USY﹣Al2 O3 hydro﹣upgrading catalysts using USY and different a﹣mount of Beta zeolite as acid components were prepared by co﹣impregnation. The catalysts were charac﹣terized by BET,FT﹣IR and NH3﹣TPD. The hydro﹣upgrading performance of the catalysts was investi﹣gated in a 100 mL high pressure trickle﹣bed reactor. The effect of Beta zeolite addition on the acidity of the catalysts with the same amount of USY and the hydroupgrading performance were tested. The re﹣sults show that the Bronsted∕Lewis ratio and total acidity of the catalysts increase with the adding amount of Beta zeolite rising. Ni﹣W∕Beta﹣USY﹣Al2 O3 catalysts reveal a high hydroupgrading activity. Under the conditions of 10. 0 MPa,H2∕oil ratio of 700∶1 and 380 ℃in upgrading zone,the diesel yield is about 90%,density is lowered by 0. 1 g∕cm3 ,sulfur content is less than 10 !g∕g,cetane number in﹣creases 19—22 units and condensation point declines dramatically.%采用Beta分子筛与USY分子筛复配作为催化剂酸性组分,利用共浸渍法制备不同Beta分子筛含量的NiW∕Beta﹣USY﹣Al2 O3系列柴油加氢改质催化剂,运用BET、FT﹣IR 和NH3﹣TPD等分析手段对催化剂进行表征;在100 mL固定床高压加氢反应器进行催化剂的加氢改质活性评价,考察Beta分子筛的加入对催化剂酸性和加氢改质催化剂活性的影响。结果表明:随Beta 分子筛加入量的增加,催化剂中B酸量∕L 酸量比值增大,总酸量增大;在压力10.0 MPa、氢油体积比700、改质段反应温度380℃的条件下,NiW∕Beta﹣USY﹣Al2 O3系列催化剂表现出良好的加氢改质性能,在柴油收率保持90%的条件下其密度(20℃)降低约0.1 g∕cm3、硫质量分数低于10!g∕g、十六烷值提高19~22个单位,凝点大幅下降。

  15. The annihilation of ortho-positronium in the {alpha} and {beta} cavities of the 4A zeolite and those CoZ4A and MnZ4A; La aniquilacion del orto-positronio en las cavidades {alpha} y {beta} de la zeolita 4A y en las de CoZ4A y MnZ4A

    Energy Technology Data Exchange (ETDEWEB)

    Cabral P, A.; Garcia S, I.; Jimenez B, J.; Solache R, M.; Bonifacio M, J.; Rodriguez F, C.; Bulbulian, S. [Instituto Nacional de Investigaciones Nucleares, A.P. 18-1027, 11801 Mexico D.F. (Mexico)

    2002-07-01

    The lifetime of the ortho-positronium in the zeolite 4A, partially dehydrated, changes to three characteristic modes. The first mode could be associated with the water elimination of the small {beta} cavity of this zeolite. At the end of this first dehydration process it is estimated a cavity radius, R = 33.8 nm. The other two types of variation of lifetime of ortho-positronium would be associated with the water elimination of the {alpha} great cavity and of the rest of the zeolite. From the zeolite 4A totally dehydrated and of the zeolite 4A exchanged with Co (II) and MN (II), also dehydrated radius are respectively determined for the {alpha} great cavity of R = 48.1, 54.5 and 56.5 nm. (Author)

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

    Directory of Open Access Journals (Sweden)

    P. C. Zonetti

    2013-12-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2013-10-15

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

  18. Selective synthesis and characterization of single-site HY zeolite-supported rhodium complexes and their use as catalysts for ethylene hydrogenation and dimerization

    Science.gov (United States)

    Khivantsev, Konstantin

    Single-site Rh(CO)2, Rh(C2H4)2 and Rh(NO)2 complexes anchored on various dealuminated HY zeolites can be used as precursors for the selective surface mediated synthesis of well-defined site-isolated Rh(CO)(H)x complexes. DFT calculations and D 2 isotope exchange experiments provide strong evidence for the formation of a family of site isolated mononuclear rhodium carbonyl hydride complexes (including the first examples of RhH complexes with undissociated H2 ligands): Rh(CO)(H2), Rh(CO)(H)2, and Rh(CO)(H). The fraction of each individual complex formed varies significantly with the Si/Al ratio of the zeolite and the nature of the precursor used. HY zeolite-supported mononuclear Rh(CO)2 complexes are very active in ethylene hydrogenation and ethylene dimerization under ambient conditions. There is strong evidence for the cooperation mechanism between mononuclear rhodium complexes and Bronsted acid sites of the zeolite support in C-C bond formation process, as well as ethane formation. Finally, it is shown that the dimerization pathway selectivity can be progressively tuned (and completely switched off) by modifying the number of Bronsted acid sites on the zeolite surface. HY zeolite-supported mononuclear Rh(NO)2 complexes can be selectively formed upon exposure of Rh(CO)2/HY to the gas phase NO/He. They are structurally similar to Rh(CO)2/HY with Rh(I) retaining square planar geometry and nitrosyl ligands adopting a linear configuration. Rh(NO)2/HY30 is active in ethylene hydrogenation and ethylene dimerization under ambient conditions. This is the first unprecedented example of a supported transition-metal nitrosyl complex capable of performing a catalytic reaction. Moreover, this is the first example of a site-isolated Rh complex with ligands other than ethylene or carbonyl, which can catalyze both ethylene hydrogenation and dimerization. Unlike its dicarbonyl counterpart, dinitrosyl rhodium complex has a uniquely different reactivity towards ethylene and hydrogen

  19. Hexane cracking over steamed phosphated zeolite H-ZSM-5: promotional effect on catalyst performance and stability.

    Science.gov (United States)

    van der Bij, Hendrik E; Meirer, Florian; Kalirai, Sam; Wang, Jian; Weckhuysen, Bert M

    2014-12-15

    The nature behind the promotional effect of phosphorus on the catalytic performance and hydrothermal stability of zeolite H-ZSM-5 has been studied using a combination of (27) Al and (31) P MAS NMR spectroscopy, soft X-ray absorption tomography and n-hexane catalytic cracking, complemented with NH3 temperature-programmed desorption and N2 physisorption. Phosphated H-ZSM-5 retains more acid sites and catalytic cracking activity after steam treatment than its non-phosphated counterpart, while the selectivity towards propylene is improved. It was established that the stabilization effect is twofold. First, the local framework silico-aluminophosphate (SAPO) interfaces, which form after phosphatation, are not affected by steam and hold aluminum atoms fixed in the zeolite lattice, preserving the pore structure of zeolite H-ZSM-5. Second, the four-coordinate framework aluminum can be forced into a reversible sixfold coordination by phosphate. These species remain stationary in the framework under hydrothermal conditions as well. Removal of physically coordinated phosphate after steam-treatment leads to an increase in the number of strong acid sites and increased catalytic activity. We propose that the improved selectivity towards propylene during catalytic cracking can be attributed to local SAPO interfaces located at channel intersections, where they act as impediments in the formation of bulky carbenium ions and therefore suppress the bimolecular cracking mechanism.

  20. Performance of ultrasonic – Treated nano-zeolites employed in the preparation of dimethyl ether

    Directory of Open Access Journals (Sweden)

    Sanaa M. Solyman

    2013-06-01

    Full Text Available Catalytic dehydration of methanol to dimethyl ether was carried out over nano-zeolites and their modified samples via ultrasonic technique. Parent H-Beta and Parent H-Mordenite zeolites are used as synthesized and after sonication. H-Mordenite sonicated for 20 and 120 min whereas H-Beta sonicated for 20 min only. The reaction temperature was varied between 100 and 225 °C at three different contact times. The different catalyst samples were characterized using: XRD, FTIR, TEM, SEM and NH3-TPD techniques. The results revealed that sonication of parent zeolite samples affects on the unit cell dimensions and their crystal size. FTIR-spectroscopic analysis indicated that sonication may decrease the pore opening and cause framework structure defects. TEM and SEM micrographs showed that sonication broke-up and re-ordered zeolite crystals with longer time resulted in a different morphology relative to parents and also change the particle size. Sonicated samples have a good performance in methanol dehydration with complete conversion and complete selectivity to dimethyl ether at lower temperature relative to the corresponding parent zeolites. TPD results indicated that the concentration of strong acid sites decreased in sonicated H-Mordenite samples leading to an increase of their catalytic activity and the selectivity to DME. On the other hand, ultrasonic treatment of H-Beta sample decreased its catalytic activity.

  1. Mesoporous Fe-containing ZSM-5 zeolite single crystal catalysts for selective catalytic reduction of nitric oxide by ammonia

    DEFF Research Database (Denmark)

    Kustov, Arkadii; Egeblad, Kresten; Kustova, Marina;

    2007-01-01

    Mesoporous and conventional Fe-containing ZSM-5 catalysts (0.5–8 wt% Fe) were prepared using a simple impregnationmethod and tested in NO selective catalytic reduction (SCR) with NH3. It was found that mesoporous Fe-ZSM-5 catalysts exhibit higher SCR activities than comparable conventional cataly...

  2. Catalysis with hierarchical zeolites

    DEFF Research Database (Denmark)

    Holm, Martin Spangsberg; Taarning, Esben; Egeblad, Kresten

    2011-01-01

    topic. Until now, the main reason for developing hierarchical zeolites has been to achieve heterogeneous catalysts with improved performance but this particular facet has not yet been reviewed in detail. Thus, the present paper summaries and categorizes the catalytic studies utilizing hierarchical...

  3. Modelling of the partial oxidation of {alpha}, {beta}-unsaturated aldehydes on Mo-V-oxides based catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Boehnke, H.; Petzoldt, J.C.; Stein, B.; Weimer, C.; Gaube, J.W. [Technische Univ. Darmstadt (Germany). Inst. fuer Chemische Technologie

    1998-12-31

    A kinetic model based on the Mars-van Krevelen mechanism that allows to describe the microkinetics of the heterogeneously catalysed partial oxidation of {alpha}, {beta}-unsaturated aldehydes is presented. This conversion is represented by a network, composed of the oxidation of the {alpha}, {beta}-unsaturated aldehyde towards the {alpha}, {beta}-unsaturated carboxylic acid and the consecutive oxidation of the acid as well as the parallel reaction of the aldehyde to products of deeper oxidation. The reaction steps of aldehyde respectively acid oxidation and catalyst reoxidation have been investigated separately in transient experiments. The combination of steady state and transient experiments has led to an improved understanding of the interaction of the catalyst with the aldehyde and the carboxylic acids as well as to a support of the kinetic model assumptions. (orig.)

  4. HYDROGENATION OF POLYCYCLIC AROMATIC COMPOUNDS USING NI SUPPORT ON H-BETA ZEOLITE IN SUPERCRITICAL CARBON DIOXIDE

    Science.gov (United States)

    The primary rationale for use of supercritical carbon dioxide as a solvent in hydrogenation is the elimination of mass transfer limitations, through enhancement of the solubility of hydrogen at the reaction locus. Hydrogenation of anthracene was performed using NiHB-zeolite catal...

  5. Hβ AND MODIFIED Hβ ZEOLITES AS CATALYSTS FOR BECKMANN REARRANGEMENT OF CYCLOHEXANONE OXIME%Hβ及改性Hβ分子筛催化环己酮肟重排制己内酰胺

    Institute of Scientific and Technical Information of China (English)

    章永洁; 王亚权; 卜亿峰; 王莅; 米镇涛; 何菲; 吴魏; 闵恩泽; 傅送保; 朱泽华

    2004-01-01

    The Beckmann rearrangement of cyclohexanone oxime is an important reaction for obtaining ε-caprolactam, the raw material of nylon 6 fibers. Currently, the widely used technologies for the production of cyclohexanone oxime produce large amounts of byproducts. For the Beckmann rearrangement, many solid acid catalysts such as alumina, boria-alumina, and zeolites including Y, those with MFI-structure and β have been studied. However, no generally accepted understanding about the reaction mechanism has been achieved.

  6. The effect of soot on ammonium nitrate species and NO2 selective catalytic reduction over Cu-zeolite catalyst-coated particulate filter.

    Science.gov (United States)

    Mihai, Oana; Tamm, Stefanie; Stenfeldt, Marie; Olsson, Louise

    2016-02-28

    interacting with the ammonium nitrate species on the CuxOy or other copper species on the surface of the zeolite particles, which reduces the ammonium nitrate blocking of the catalyst and thereby results in higher NO2 SCR activity.

  7. {gamma} alumina- and HY zeolite-supported molybdenum catalysts: characterisation of the oxidic and sulfided phases; Catalyseurs a base de molybdene supporte sur alumine {gamma} et zeolithe HY: caracterisation des phases oxydes et sulfures

    Energy Technology Data Exchange (ETDEWEB)

    Plazenet, G.

    2001-10-01

    Oxidic precursors of hydro-treatment catalysts (Co)Mo/alumina or zeolite were characterised by Raman spectroscopy, NMR and EXAFS at the Mo and Co K-edges. The formation of an Anderson-type alumino-molybdate compound upon impregnation of the support with an ammonium hepta-molybdate solution was confirmed for alumina, and also observed for the HY zeolitic support, with consumption of the amorphous alumina of the zeolite. In absence of the latter, ammonium hepta-molybdate precipitates. The species are conserved upon drying; upon calcination, the alumino-molybdate evolves into a surface aluminium molybdate type phase, whereas the hepta-molybdate transforms into MoO{sub 3}. The species formed upon impregnation are located in the inter-granular porosity whereas MoO{sub 3} vapor-condensation leads to formation of dimers located inside the zeolitic structure. The study of the cobalt-promoted precursors showed that the evolution of the molybdenum is the same in the case of co-impregnation preparation. Impregnation with cobalt-molybdate prevents the formation of the alumino-molybdate anion and thus enables the preservation of the Mo-Co interaction but, whatever the precursor, the leveling effect of the calcination-re-hydration steps was demonstrated. An EXAFS study at different sulfur coverages of the MoS{sub 2} platelets in the alumina-supported sulfided catalysts showed the limitations of EXAFS for size determination of MoS{sub 2} crystallites, a parameter that can be reached by AWAXS, which also conveys information about sheet-stacking. The EXAFS study of sulfided (Co)Mo/HY systems revealed incomplete sulfidation of the samples and the very high dispersion of the active phase. The absence of an observable Mo-Co interaction whatever the preparation of the promoted catalysts is consistent with the absence of promoting effect in toluene hydrogenation. (author)

  8. Synthesis and testing of nanosized zeolite Y

    Science.gov (United States)

    Karami, Davood

    This work focuses on the synthesis and testing of nanosized zeolite Y. The synthesis formulations of faujasite-type structure of zeolite Y prepared in nanosized form are described. The synthetic zeolite Y is the most widely employed for the preparation of fluid catalytic cracking (FCC) catalysts. The synthesis of zeolite Y is very complicated process. The mean particle size of zeolite Y is 1800 nm. The major challenge of this work involved reducing this average particle size to less than 500 nm. The preliminary experiments were conducted to obtain the pure zeolite Y using the soluble silicates as a silica source. This was achieved by applying the experimental design approach to study the effects of many parameters. The ageing time turned out to be the most significant variable affecting product purity. Based on the preliminary results, a detailed investigation was carried out to determine the effects of silica-alumina precursor preparations on zeolite Y synthesis. Aluminosilicate precursors were prepared by gelling and precipitation of soluble silicate. The as-prepared precursors were used for the hydrothermal synthesis of zeolite Y. The procedure of the precipitation of soluble silicate yielded pure zeolite Y at the conventional synthesis conditions. The extent of purity of zeolite Y depends on the surface areas of aluminosilicate precursors. A novel approach to zeolite Y synthesis was employed for the preparation of the pure nanosized zeolite Y. This was achieved by applying the method of impregnation of precipitated silica. This novel method of impregnation for zeolite Y preparation allows eliminating the vigorous agitation step required for the preparation of a homogeneous silica solution, thereby simplifying the synthesis of zeolite Y in one single vessel. In case of the synthesis of nanosized zeolite Y, the effect of varying the organic templates on the formation of nanosized particles of zeolite Y was investigated, while all other reaction parameters were

  9. Highly selective Lewis acid sites in desilicated MFI zeolites for dihydroxyacetone isomerization to lactic acid.

    Science.gov (United States)

    Dapsens, Pierre Y; Mondelli, Cecilia; Pérez-Ramírez, Javier

    2013-05-01

    Desilication of commercial MFI-type (ZSM-5) zeolites in solutions of alkali metal hydroxides is demonstrated to generate highly selective heterogeneous catalysts for the aqueous-phase isomerization of biobased dihydroxyacetone (DHA) to lactic acid (LA). The best hierarchical ZSM-5 sample attains a LA selectivity exceeding 90 %, which is comparable to that of the state-of-the-art catalyst (i.e., the Sn-beta zeolite); this optimized hierarchical catalyst is recyclable over three runs. The Lewis acid sites, which are created through desilication along with the introduction of mesoporosity, are shown to play a crucial role in the formation of the desired product; these cannot be achieved by using other post-synthetic methods, such as steaming or impregnation of aluminum species. Desilication of other metallosilicates, such as Ga-MFI, also leads to high LA selectivity. In the presence of a soluble aluminum source, such as aluminum nitrate, alkaline-assisted alumination can introduce these unique Lewis acid centers in all-silica MFI zeolites. These findings highlight the potential of zeolites in the field of biomass-to-chemical conversion, and expand the applicability of desilication for the generation of selective catalytic centers.

  10. A Green Synthesis of 2-Ethylanthraquinone by Dehydration of 2-(4'-ethylbenzoyl) benzoic Acid over Solid Acid Catalysts

    Institute of Scientific and Technical Information of China (English)

    Ren Shu XU; Xin Wen GUO; Gui Ru WANG; Zhu Xia ZHANG

    2005-01-01

    The dehydration of 2-(4'-ethylbenzoyl) benzoic acid (BE acid) to 2-ethylanthraquinone(2-EAQ) was investigated over solid acid catalysts. The results showed that H-beta zeolite catalyst modified by dilute HNO3 solution exhibited an excellent performance. In our study, theconversion of BE acid can reach 96.7%, and the selectivity to 2-EAQ is up to 99.6%.

  11. Incorporação de dióxido de titânio em zeólitas para emprego em fotocatálise heterogênea Titanium oxide incorporation on zeolites for heterogeneous photocatalisis

    Directory of Open Access Journals (Sweden)

    Jean C. Merg

    2010-01-01

    Full Text Available This work proposes the study of heterogeneous photocatalysis using TiO2 impregnated in zeolites beta, ZSM-5, mordenite, NaXb, NaXp and NaY for the decomposition of methylene blue. The catalysts were characterized by XRD, IR, textural analyses by N2 adsorption, SEM, DRS and the reaction of decomposition was monitored by UV visible. The results indicated that didn't have structural changes in the catalysts after Ti impregnations, only in the case of NaY and NaX zeolites. The better photocatalyst to metylene blue decomposition was beta/Ti zeolite due had one structure more accessible (with bigger porous helping in TiO2 dispersion and catalytic active.

  12. Para-Xylene Maximization Part VIII: Promotion of H-ZSM-5 Zeolite by Pt and HF Doping for Use as Catalysts in Toluene Alkylation with Methanol

    Institute of Scientific and Technical Information of China (English)

    Ahmed K.ABOUL-GHEIT; Ateyya A.ABOUL-ENEIN; Ahmed E.AWADALLAH; Salwa A.GHONEIM; Eman A.EMAM

    2010-01-01

    Toluene was alkylated with methanol in a flow type reactor at temperatures between 300 and 500℃ using H-ZSM-5 zeolite, 0.2%Pt/H-ZSM-5 and hydrofluorinated 0.2%Pt/H-ZSM-5 with HF concentrations of 1.0%, 2.0%, 3.0%, or 4.0%. Pt primarily enhances toluene conversion, total xylenes production, and p-xylene relative to its thermodynamic equilibrium. As the concentration of HF increases from 1.0% to 3.0%, the catalyst activity increases because of the increase in the number of acid sites and their strength. Additionally, the surface area and Pt dispersion also increases. An advantage of increased HF doping is that the formation of voluminous trimethylbenzene (TMB) byproducts is inhibited. However, at a HF concentration of 4.0%, AI and Si are partially leached and then deposited mostly in the wider catalytic pores. This was determined by evaluating the pore volume distribution and we determined that reactivity inhibition was ob-viously present and was due to diffusion restriction.

  13. Oxide acid-base reaction relating to the inhibition of vandium attack on REY zeolite catalysts. [Rare earth-exchanged yttrium

    Energy Technology Data Exchange (ETDEWEB)

    Jones, R.L. (Naval Research Lab., Washington, D.C. (USA))

    1991-05-01

    Certain materials, especially Sn, passivate the rare earth-exchanged Y zeolite (REY) used in petrochemical fluid-cracking catalysts against vanadium degradation caused by V impurities in the feed oil. The mechanism of passivation was investigated here from the standpoint of high-temperature oxide acid-base reaction; i.e., where the controlling factors were considered to be Lewis acid-base reactions between V{sub 2}O{sub 5}, the RE oxides, SnO{sub 2}, etc. Molten salt tests at 680{degree}C showed SnO{sub 2}, presumably because of its acidic nature, to be essentially nonreactive with V{sub 2}O{sub 5} or Na{sub 2}O-V{sub 2}O{sub 5} compounds. A hypothesis was developed to explain how the passivation effect by Sn might result from the unique resistivity of SnO{sub 2} to reaction with V{sub 2}O{sub 5}.

  14. Zeolites and Zeotypes for Oil and Gas Conversion

    NARCIS (Netherlands)

    Vogt, Eelco T C; Whiting, Gareth T.; Dutta Chowdhury, Abhishek; Weckhuysen, Bert M.|info:eu-repo/dai/nl/285484397

    2015-01-01

    Zeolite-based catalyst materials are widely used in chemical industry. In this chapter, the applications of zeolites and zeotypes in the catalytic conversion of oil and gas are reviewed. After a general introduction to zeolite science and technology, we discuss refinery applications, such as fluid c

  15. Study on Synthesis and Catalytic Performance of Hierarchical Zeolite

    Institute of Scientific and Technical Information of China (English)

    Zhang Lingling; Li Fengyan; ZhaoTianbo; Sun Guida

    2007-01-01

    A kind of hierarchical zeolite catalyst was synthesized by hydrothermal method.X-ray diffraction (XRD)and nitrogen adsorption-desorption method were used to study the phase and aperture structure of the prepared catalyst.Infrared(IR)spectra of pyridine adsorbed on the sample showed that the hierarchical zeolite really had much more Bronsted and Lewis acidic sites than the HZSM-5 zeolite.The catalytic cracking of large hydrocarbon molecules showed that the hierarchical zeolite had a higher catalytic activity than the HZSM-5 zeolite.

  16. 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.

  17. Zeolitic catalytic conversion of alochols to hydrocarbons

    Energy Technology Data Exchange (ETDEWEB)

    Narula, Chaitanya K.; Davison, Brian H.; Keller, Martin

    2017-01-03

    A method for converting an alcohol to a hydrocarbon, the method comprising contacting said alcohol with a metal-loaded zeolite catalyst at a temperature of at least 100.degree. C. and up to 550.degree. C., wherein said alcohol can be produced by a fermentation process, said metal is a positively-charged metal ion, and said metal-loaded zeolite catalyst is catalytically active for converting said alcohol to said hydrocarbon.

  18. Highly efficient synthesis of dimethyl ether from syngas over the admixed catalyst of CuO-ZnO-Al{sub 2}O{sub 3} and antimony oxide modified HZSM-5 zeolite

    Energy Technology Data Exchange (ETDEWEB)

    Mao Dongsen, E-mail: dsmao1106@yahoo.com.c [Research Institute of Applied Catalysis, Department of Chemical Engineering, Shanghai Institute of Technology, Shanghai 200235 (China); Xia Jianchao; Zhang Bin [Shanghai Research Institute of Petrochemical Technology, SINOPEC, Shanghai 201208 (China); Lu Guanzhong [Research Institute of Applied Catalysis, Department of Chemical Engineering, Shanghai Institute of Technology, Shanghai 200235 (China)

    2010-06-15

    A series of HZSM-5 zeolites modified with various contents of antimony oxide (0-30 wt.%) were prepared by solid state ion reaction at 500 deg. C, and the acidities of the resulted materials were characterized by temperature-programmed desorption of NH{sub 3}. The direct synthesis of dimethyl ether (DME) from syngas was carried out over the admixed catalysts of an industrial CuO-ZnO-Al{sub 2}O{sub 3} methanol synthesis catalyst and the parent and antimony oxide modified HZSM-5 zeolites under pressurized fixed-bed continuous flow conditions. The results indicated that modification of HZSM-5 with suitable amount of antimony oxide significantly decreased the selectivity for undesired byproducts like hydrocarbons and carbon dioxide from 9.3% and 32.4% to less than 1% and 28%, respectively, so the selectivity for DME was enhanced greatly from 55% to 69% under temperature of 260 deg. C, pressure of 4 MPa and gas hourly space velocity of 1500 mL h{sup -1} g{sub cat}{sup -1}. The decrease in the formation of hydrocarbons and carbon dioxide can be attributed to the significant decline in the amount of strong acid sites of the HZSM-5 zeolite induced by antimony oxide modification. Additionally, the influences of the operating parameters on the performance of the most efficient catalyst were also investigated. The results showed that high reaction temperature and high gas hourly space velocity resulted in both lower carbon monoxide conversion and lower dimethyl ether selectivity, so they should be no higher than 280 deg. C and 3000 mL h{sup -1} g{sub cat}{sup -1}, respectively.

  19. Highly efficient synthesis of dimethyl ether from syngas over the admixed catalyst of CuO-ZnO-Al{sub 2}O{sub 3} and antimony oxide modified HZSM-5 zeolite

    Energy Technology Data Exchange (ETDEWEB)

    Dongsen Mao; Guanzhong Lu [Research Institute of Applied Catalysis, Department of Chemical Engineering, Shanghai Institute of Technology, Shanghai 200235 (China); Jianchao Xia; Bin Zhang [Shanghai Research Institute of Petrochemical Technology, SINOPEC, Shanghai 201208 (China)

    2010-06-15

    A series of HZSM-5 zeolites modified with various contents of antimony oxide (0-30 wt.%) were prepared by solid state ion reaction at 500 C, and the acidities of the resulted materials were characterized by temperature-programmed desorption of NH{sub 3}. The direct synthesis of dimethyl ether (DME) from syngas was carried out over the admixed catalysts of an industrial CuO-ZnO-Al{sub 2}O{sub 3} methanol synthesis catalyst and the parent and antimony oxide modified HZSM-5 zeolites under pressurized fixed-bed continuous flow conditions. The results indicated that modification of HZSM-5 with suitable amount of antimony oxide significantly decreased the selectivity for undesired byproducts like hydrocarbons and carbon dioxide from 9.3% and 32.4% to less than 1% and 28%, respectively, so the selectivity for DME was enhanced greatly from 55% to 69% under temperature of 260 C, pressure of 4 MPa and gas hourly space velocity of 1500 mL h{sup -1} g{sub cat}{sup -1}. The decrease in the formation of hydrocarbons and carbon dioxide can be attributed to the significant decline in the amount of strong acid sites of the HZSM-5 zeolite induced by antimony oxide modification. Additionally, the influences of the operating parameters on the performance of the most efficient catalyst were also investigated. The results showed that high reaction temperature and high gas hourly space velocity resulted in both lower carbon monoxide conversion and lower dimethyl ether selectivity, so they should be no higher than 280 C and 3000 mL h{sup -1} g{sub cat}{sup -1}, respectively. (author)

  20. Fluoride-assisted synthesis of bimodal microporous SSZ-13 zeolite.

    Science.gov (United States)

    Zhu, Xiaochun; Kosinov, Nikolay; Hofmann, Jan P; Mezari, Brahim; Qian, Qingyun; Rohling, Roderigh; Weckhuysen, Bert M; Ruiz-Martínez, Javier; Hensen, Emiel J M

    2016-02-21

    The presence of small amount of fluoride in alkaline hydrothermal synthesis of SSZ-13 zeolite yields bimodal microporous particles with substantially improved performance in the methanol-to-olefins (MTO) reaction. Hydrocarbon uptake measurements and fluorescence microspectroscopy of spent catalysts demonstrate enhanced diffusion through micropores at the grain boundaries of nanocrystals running through the zeolite particles. Fluoride-assisted SSZ-13 synthesis is a cheap and scalable approach to optimize the performance of MTO zeolite catalysts.

  1. Xylose isomerization with zeolites in a two-step alcohol-water process.

    Science.gov (United States)

    Paniagua, Marta; Saravanamurugan, Shunmugavel; Melian-Rodriguez, Mayra; Melero, Juan A; Riisager, Anders

    2015-03-01

    Isomerization of xylose to xylulose was efficiently catalyzed by large-pore zeolites in a two-step methanol-water process that enhanced the product yield significantly. The reaction pathway involves xylose isomerization to xylulose, which, in part, subsequently reacts with methanol to form methyl xyluloside (step 1) followed by hydrolysis after water addition to form additional xylulose (step 2). NMR spectroscopy studies performed with (13) C-labeled xylose confirmed the proposed reaction pathway. The most active catalyst examined was zeolite Y, which proved more active than zeolite beta, ZSM-5, and mordenite. The yield of xylulose obtained over H-USY (Si/Al=6) after 1 h of reaction at 100 °C was 39%. After water hydrolysis in the second reaction step, the yield increased to 47%. Results obtained from pyridine adsorption studies confirm that H-USY (6) is a catalyst that combines Brønsted and Lewis acid sites, and isomerizes xylose in alcohol media to form xylulose at low temperature. The applied zeolites are commercially available; do not contain any auxiliary tetravalent metals, for example, tin, titanium, or zirconium; isomerize xylose efficiently; are easy to regenerate; and are prone to recycling.

  2. Nano Catalysts for Diesel Engine Emission Remediation

    Energy Technology Data Exchange (ETDEWEB)

    Narula, Chaitanya Kumar [ORNL; Yang, Xiaofan [ORNL; Debusk, Melanie Moses [ORNL; Mullins, David R [ORNL; Mahurin, Shannon Mark [ORNL; Wu, Zili [ORNL

    2012-06-01

    The objective of this project was to develop durable zeolite nanocatalysts with broader operating temperature windows to treat diesel engine emissions to enable diesel engine based equipment and vehicles to meet future regulatory requirements. A second objective was to improve hydrothermal durability of zeolite catalysts to at least 675 C. The results presented in this report show that we have successfully achieved both objectives. Since it is accepted that the first step in NO{sub x} conversion under SCR (selective catalytic reduction) conditions involves NO oxidation to NO{sub 2}, we reasoned that catalyst modification that can enhance NO oxidation at low-temperatures should facilitate NO{sub x} reduction at low temperatures. Considering that Cu-ZSM-5 is a more efficient catalyst than Fe-ZSM-5 at low-temperature, we chose to modify Cu-ZSM-5. It is important to point out that the poor low-temperature efficiency of Fe-ZSM-5 has been shown to be due to selective absorption of NH{sub 3} at low-temperatures rather than poor NO oxidation activity. In view of this, we also reasoned that an increased electron density on copper in Cu-ZSM-5 would inhibit any bonding with NH{sub 3} at low-temperatures. In addition to modified Cu-ZSM-5, we synthesized a series of new heterobimetallic zeolites, by incorporating a secondary metal cation M (Sc{sup 3+}, Fe{sup 3+}, In{sup 3+}, and La{sup 3+}) in Cu exchanged ZSM-5, zeolite-beta, and SSZ-13 zeolites under carefully controlled experimental conditions. Characterization by diffuse-reflectance ultra-violet-visible spectroscopy (UV-Vis), X-ray powder diffraction (XRD), extended X-ray absorption fine structure spectroscopy (EXAFS) and electron paramagnetic resonance spectroscopy (EPR) does not permit conclusive structural determination but supports the proposal that M{sup 3+} has been incorporated in the vicinity of Cu(II). The protocols for degreening catalysts, testing under various operating conditions, and accelerated aging

  3. Towards a full understanding of the nature of Ni(II) species and hydroxyl groups over highly siliceous HZSM-5 zeolite supported nickel catalysts prepared by a deposition-precipitation method.

    Science.gov (United States)

    Chen, Bao-Hui; Chao, Zi-Sheng; He, Hao; Huang, Chen; Liu, Ya-Juan; Yi, Wen-Jun; Wei, Xue-Ling; An, Jun-Fang

    2016-02-14

    Highly siliceous HZSM-5 zeolite supported nickel catalysts prepared by a deposition-precipitation (D-P) method were characterized by Fourier transform infrared (FT-IR), hydrogen temperature programmed reduction (H2-TPR), X-ray diffraction (XRD), N2-absorption/desorption, field emission scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), and (27)Al magic-angle nuclear magnetic resonance (MAS NMR) techniques. The results showed that the D-P of nickel species occurred predominantly on the internal surface of highly siliceous HZSM-5 zeolite, in which the internal silanol groups located on the hydroxylated mesopores or nanocavities played a key role. During the D-P process, nickel hydroxide was first deposited-precipitated via olation/polymerization of neutral hydroxoaqua nickel species over the HZSM-5 zeolite. With the progress of the D-P process, 1 : 1 nickel phyllosilicate was formed over the HZSM-5 via the hetero-condensation/polymerization between charged hydroxoaqua nickel species and monomer silicic species generated due to the partial dissolution of the HZSM-5 framework. The 1 : 1 nickel phyllosilicate could also be generated via the hydrolytic adsorption of hydroxoaqua nickel species and their subsequent olation condensation. After calcination, the deposited-precipitated nickel hydroxide was decomposed into nickel oxide, while the 1 : 1 nickel phyllosilicate was transformed into 2 : 1 nickel phyllosilicate. According to the above mechanism, Ni(ii) species were present both in the form of nickel oxide and 2 : 1 nickel phyllosilicate, which were mutually separated from each other, being highly dispersed over HZSM-5 zeolite.

  4. Kinetics of zeolite dealumination in steam

    Energy Technology Data Exchange (ETDEWEB)

    Hughes, C.D.; Labouriau, A.; Crawford, S.N.; Romero, R.; Quirin, J.; Earl, W.L.

    1998-08-01

    Zeolite dealumination is a well known phenomenon that contributes to the deactivation or activation of catalysts in several different applications. The most obvious effect is in acid catalysis where dealumination under reaction conditions removes the Broensted sites, thus deactivating the catalyst. The authors are interested in the use of cation exchanged zeolites as selective reduction catalysts for removal of NO{sub x} from exhaust streams, particularly from automotive exhaust. In this case, copper exchanged ZSM-5 has been shown to be an effective catalyst for the generic reaction of NO{sub x} with hydrocarbons. However, high temperature and steam in combustion exhaust causes dealumination and consequent migration of copper out of the zeolite structure resulting in rapid deactivation of the catalyst. Dealumination of zeolites has been reported by many authors in uncountable papers and cannot be reviewed here. However, to the authors` knowledge there are no reports on the kinetics of dealumination under varying conditions of temperature and steam. By measuring the kinetics of dealumination with different zeolites and exchange cations they expect to develop working models of the dealumination process that will allow control of zeolite deactivation. This manuscript is a description of the basic techniques used and a progress report on the very beginning of this study.

  5. Esterification of Free Fatty Acids in Waste Cooking Oil by Heterogeneous Catalysts

    Institute of Scientific and Technical Information of China (English)

    刘丽艳; 刘志敏; 唐国武; 谭蔚

    2014-01-01

    Waste cooking oil (WCO) is becoming the most promising alternative feedstock to produce biodiesel due to its low cost in China. In this study, NKC-9 ion-exchange resin and H-beta zeolite were selected as heterogeneous catalysts in the WCO esterification process and their esterification characteristics were compared by orthogonal ex-periments. NKC-9 resin showed higher activity and achieved a higher final conversion compared with H-beta zeolite under the same reaction conditions. Reusability experiments showed that NKC-9 resin still exhibited high activity after 5 runs. The effects of the mole ratio of alcohol to oil, reaction time, reaction temperature and the catalyst dose were investigated by multifactor orthogonal analysis. The influence of the free fatty acid (FFA) content was also investi-gated, and the result showed that the esterification rate could be as high as 98.4%when the FFA content was 6.3wt%.

  6. Nanostructured Basic Catalysts: Opportunities for Renewable Fuels

    Energy Technology Data Exchange (ETDEWEB)

    Conner, William C; Huber, George; Auerbach, Scott

    2009-06-30

    This research studied and developed novel basic catalysts for production of renewable chemicals and fuels from biomass. We focused on the development of unique porous structural-base catalysts zeolites. These catalysts were compared to conventional solid base materials for aldol condensation, that were being commercialized for production of fuels from biomass and would be pivotal in future biomass conversion to fuels and chemicals. Specifically, we had studied the aldolpyrolysis over zeolites and the trans-esterification of vegetable oil with methanol over mixed oxide catalysts. Our research has indicated that the base strength of framework nitrogen in nitrogen substituted zeolites (NH-zeolites) is nearly twice as strong as in standard zeolites. Nitrogen substituted catalysts have been synthesized from several zeolites (including FAU, MFI, BEA, and LTL) using NH3 treatment.

  7. Effects of Hydrothermal Aging on NH3-SCR reaction over Cu/zeolites

    Energy Technology Data Exchange (ETDEWEB)

    Kwak, Ja Hun; Tran, Diana N.; Burton, Sarah D.; Szanyi, Janos; Lee, Jong H.; Peden, Charles HF

    2012-02-06

    The effects of hydrothermal treatment on model Cu/zeolite catalysts were investigated to better understand the nature of Cu species for the selective catalytic reduction of NO{sub x} by NH{sub 3}. After hydrothermal aging at 800 C for 16 h, the NO{sub x} reduction performance of Cu-ZSM-5 and Cu-beta were significantly reduced at low temperatures, while that of Cu-SSZ-13 was not affected. When the zeolite framework aluminum species were probed using solid state {sup 27}Al-NMR, significant reduction in the intensities of the tetrahedral aluminum peak was observed for Cu-ZSM-5 and Cu-beta, although no increase in the intensities of the octahedral aluminum peak was observed. When the redox behavior of Cu species was examined using H{sub 2}-TPR, it was found that Cu{sup 2+} could be reduced to Cu{sup +} and to Cu{sup 0} fir Cu-ZSM-5 and Cu-beta catalysts, while Cu{sup 2+} could be reduced to Cu{sup +} only for Cu-SSZ-13. After hydrothermal aging, CuO and Cu-aluminate species were found to form in Cu-ZSM-5 and Cu-beta, while little changes were observed for Cu-SSZ-13.

  8. Application of novel Polypyrrole/thiol-functionalized zeolite Beta/MCM-41 type mesoporous silica nanocomposite for adsorption of Hg2+ from aqueous solution and industrial wastewater: Kinetic, isotherm and thermodynamic studies

    Science.gov (United States)

    Javadian, Hamedreza; Taghavi, Mehdi

    2014-01-01

    Hierarchical zeolite consists of both microporous and unordered mesoporous structures. A composite of Polypyrrole/thiol-functionalized Beta/MCM-41 (PPy/SH-Beta/MCM-41) was prepared, characterized by FE-SEM, FT-IR, XRD, TGA and BET analysis and applied in the investigation of its adsorption characteristics for the removal of Hg2+ ions from aqueous solutions. Thiol-functionalized Beta/MCM-41 (SH-Beta/MCM-41) was prepared by 3-mercaptopropyltrimethoxysilane (MPTMS) in the presence of aerosil-200 as a silica source by two-step hydrothermal crystallization procedure. Batch mode experiments were conducted and three kinetic models were used to describe the adsorption process. The experimental data fitted very well with the Pseudo-second-order kinetic model. The calculated thermodynamic parameters (ΔH, ΔS and ΔG) revealed that the adsorption of Hg2+ onto PPy/SH-Beta/MCM-41 is an endothermic and spontaneous process. It was found that temperature has a positive effect on the removal efficiency and that PPy/SH-Beta/MCM-41 is potentially able to remove Hg2+ ions from aqueous solutions at even high concentrations (400 mg L-1). The recovery of Hg2+ from the PPy/SH-Beta/MCM-41 adsorbent was found to be more than 90% using 0.5 M H2SO4, and the ability of the absorbent to be reused for removal of Hg2+ was investigated.

  9. Functionalization of zeolitic cavities: grafting NH2 groups in framework T sites of B-SSZ-13--a way to obtain basic solids catalysts?

    Science.gov (United States)

    Regli, Laura; Bordiga, Silvia; Busco, Claudia; Prestipino, Carmelo; Ugliengo, Piero; Zecchina, Adriano; Lamberti, Carlo

    2007-10-10

    Insertion of B atoms into an Al-free zeolitic framework with CHA topology results in the formation of B-SSZ-13 zeotype with Si/B = 11. B K-edge NEXAFS testifies that B forms [B(OSi)4] units in a Td-like geometry (sp3-hybridized B atoms). According to B K-edge NEXAFS and IR, template burning results in the formation of [B(OSi)3] units in a D3h-like geometry (sp2-hybridized B atoms) with a break of a B-O-Si bond and the formation of a Si-OH group. The activated material contains B(III) Lewis acid centers able to specifically coordinate bases like NH3. Such [B(OSi)3] units are reactive toward ammonia, resulting in the formation of B-NH2 surface functionality inside the pores of B-SSZ-13 already under mild conditions, i.e., 35 mbar of NH3 at 373 K for 30 min and without crystallinity degradation. A minor fraction of Si-NH2 cannot be excluded owing to the presence of two IR doublets at 3500 and 3430 cm-1 and at 1600 and 1550 cm-1. Ab initio B3LYP/6-31+G(d,p) calculations on a cluster model, supported by a single-point MP2 on B3LYP/6-31+G(D,P) optimized structures, found the break by NH3 of a B-O-Si bond of the [B(OSi)3] unit with formation of [SiOH] and [H2N-B(OSi)2] species to be energetically favored. Comparison between experimental and computed frequency shifts shows them to be in semiquantitative agreement. The high stability of the B-NH2 surface functionality is probed by N K-edge NEXAFS spectra collected under UHV conditions. These findings can open a new route in the preparation of shape selective solid basic catalysts.

  10. Synthesis of Hydrocarbons from H2-Deficient Syngas in Fischer-Tropsch Synthesis over Co-Based Catalyst Coupled with Fe-Based Catalyst as Water-Gas Shift Reaction

    Directory of Open Access Journals (Sweden)

    Ting Ma

    2015-01-01

    Full Text Available The effects of metal species in an Fe-based catalyst on structural properties were investigated through the synthesis of Fe-based catalysts containing various metal species such, as Mn, Zr, and Ce. The addition of the metal species to the Fe-based catalyst resulted in high dispersions of the Fe species and high surface areas due to the formation of mesoporous voids about 2–4 nm surrounded by the catalyst particles. The metal-added Fe-based catalysts were employed together with Co-loaded beta zeolite for the synthesis of hydrocarbons from syngas with a lower H2/CO ratio of 1 than the stoichiometric H2/CO ratio of 2 for the Fischer-Tropsch synthesis (FTS. Among the catalysts, the Mn-added Fe-based catalyst exhibited a high activity for the water-gas shift (WGS reaction with a comparative durability, leading to the enhancement of the CO hydrogenation in the FTS in comparison with Co-loaded beta zeolite alone. Furthermore, the loading of Pd on the Mn-added Fe-based catalyst enhanced the catalytic durability due to the hydrogenation of carbonaceous species by the hydrogen activated over Pd.

  11. The effect of physical and chemical treatment on nano-zeolite characterization and their performance in dimethyl ether preparation

    Directory of Open Access Journals (Sweden)

    Sanaa M. Solyman

    2015-09-01

    Full Text Available Catalytic dehydration of methanol to dimethyl ether (DME was investigated using physically and chemically modified H-Mordenite and H-Beta zeolites as catalysts. Physical modification was carried out using ultrasonic wave’s energy, while chemical modification was performed through impregnation in aluminum nitrate followed by calcination. The produced solid catalysts were evaluated as selective catalysts for the dehydration of methanol to dimethyl ether at 100–250 °C performed at three different contact times. Chemical and structural characterizations of the solid catalysts were identified using XRD, FT-IR, TEM, SEM and NH3-TPD. Ultrasonication physical mixing of solids proved as useful tool of preparation, producing fine reordered crystals of nanocomposite zeolites with novel morphology. The newly ordered crystals were distinguished by their frame work structure, acidic properties, crystal and particle sizes, unit cell volume, pore opening, and favorable catalytic activity of 100% selectivity to DME at 200 °C for all contact times studied. The effects of Al2O3 on the dispersion and interaction within the nano-zeolite crystals and hence on the catalytic dehydration of methanol were verified as the major influence toward utmost selectivity.

  12. Diastereoselective Synthesis of trans-beta-Lactams Using a Simple Multifunctional Catalyst.

    Science.gov (United States)

    Abraham, Ciby J; Paull, Daniel H; Dogo-Isonagie, Cajetan; Lectka, Thomas

    2009-01-01

    A catalytic, highly diastereoselective process for the synthesis of trans-beta-lactams is reported. This system is based on a phosphonium fluoride precatalyst that both activates the nucleophile and directs the reaction process for high yield and diastereoselectivity.

  13. Zeolite-Based Organic Synthesis (ZeoBOS) of Acortatarin A: First Total Synthesis Based on Native and Metal-Doped Zeolite-Catalyzed Steps.

    Science.gov (United States)

    Wimmer, Eric; Borghèse, Sophie; Blanc, Aurélien; Bénéteau, Valérie; Pale, Patrick

    2017-01-31

    Similarly to polymer-supported assisted synthesis (PSAS), organic synthesis could be envisaged being performed by using zeolites, native or metal-doped, as heterogeneous catalysts. To illustrate this unprecedented Zeolite-Based Organic Synthesis (ZeoBOS), the total synthesis of acortatarin A was achieved through a novel strategy and using five out of eleven synthetic steps catalyzed by H- or metal-doped zeolites as catalysts. Notably, the formation of an yne-pyrrole intermediate with a copper-doped zeolite and the spiroketalization of an alkyne diol with a silver-doped zeolite have been developed as key steps of the synthesis.

  14. 乙醇脱水制乙烯中亚微米ZSM-5分子筛催化剂的积碳研究%Coking Behavior of Submicron ZSM-5 Zeolite Catalyst in Dehydration of Ethanol to Ethylene

    Institute of Scientific and Technical Information of China (English)

    王飞; 罗漫; 肖文德; 程晓维; 龙英才

    2011-01-01

    Reactions and coking behaviors of ethanol, diethyl ether or ethylene on a submicron ZSM-5 zeolite catalyst, which was used in dehydration of ethanol to ethylene, were studied in a fixbed reactor. The coking behavior and the dehydration mechanism were analyzed by means of TG, N2 adsorption-desorption techniques, pyridine adsorption FTIR and 13C NMR. Experimental results showed that diethyl ether was an intermediate of the ethanol dehydration to ethylene and that ethylene oligomerization was responsible for the coke formation. The coke might consist mainly of alkyl aromatics and the coke deposition rate was correlated to the olefin content and the water content in the reaction mixture. The coke deposition rate on the ZSM-5 zeolite catalyst lowered in the following order: ethylene > ethylene and water > diethyl ether > ethanol, which were used as feeds separately.After 100 h on stream, the coke deposits blocked more than 70% of the catalyst pores, and consumed more than 80% of acid sites on the catalyst, which caused a loss of catalyst activity.%在固定床反应器中研究了乙醇脱水反应中亚微米ZSM-5分子筛催化剂上乙醇、乙醚和乙烯的反应及积碳行为,采用TG、低温氮气吸附-脱附、吡啶吸附红外光谱和13C NMR等方法对催化剂进行了表征,以考察分子筛催化剂的积碳行为及乙醇脱水反应机理.实验结果表明,乙醚是乙醇脱水生成乙烯的中间体,而乙烯低聚是积碳的主要来源;积碳的主要组成可能是烷基芳烃,而积碳速率与反应混合物中的烯烃含量及水含量有关,ZSM-5分子筛催化剂上各物质积碳速率由快到慢的顺序:乙烯>乙烯+水>乙醚>乙醇;在线反应100h后,积碳堵塞了70%以上的催化剂孔道,并且消耗了80%以上的催化剂酸中心,因而导致催化剂活性有所降低.

  15. Proton Adsorption Selectivity of Zeolites in Aqueous Media: Effect of Si/Al Ratio of Zeolites

    Directory of Open Access Journals (Sweden)

    Moses Wazingwa Munthali

    2014-12-01

    Full Text Available In addition to their well-known uses as catalysts, zeolites are utilized to adsorb and remove various cations from aqueous system. The adsorption of the cations is ascribed to the negative charge of zeolites derived from isomorphous substitution of Si by Al. The amount of Na+ adsorption on 4A, X, Y, Na-P1 and mordenite type zeolites were determined in aqueous media, in a two-cation (Na+ and H+ system. Although each zeolite has a constant amount of negative charge, the amount of Na+ adsorption of each zeolite decreased drastically at low pH−pNa values, where pH−pNa is equal to log{(Na+/(H+}. By using the plot of the amount of Na+ adsorption versus pH−pNa, an index of the H+ selectivity, which is similar to the pKa of acids, of each zeolite was estimated, and the index tended to increase with decreasing Si/Al ratio of zeolites. These indicate that zeolites with lower Si/Al and higher negative charge density have higher H+ adsorption selectivity, and in fact, such a zeolite species (4A and X adsorbed considerable amount of H+ even at weakly alkaline pH region. The adsorption of H+ results in the decrease of cation adsorption ability, and may lead to the dissolution of zeolites in aqueous media.

  16. β沸石中Fe(Ⅱ)Salen络合物的合成及性能研究%SYNTHESIS AND CHARACTERIZATION OF Fe( Ⅱ )SALEN COMPLEX IN ZEOLITE BETA

    Institute of Scientific and Technical Information of China (English)

    马静红; 李瑞丰; 谢克昌

    2001-01-01

    Fe( Ⅱ )Salen( N, N',-bis(salicylaldehyde)ethylenediimine) was synthesized inside the cavity of zeolite Beta by the flexible ligand method and characterized by various physicochemical methods such as XRD, SEM, TG-DTA, UVVis. Evidences indicate by elemental analysis and thermal analysis that Fe( Ⅱ ) ion complexes stoichiometrically associated with Salen molecule in zeolite Beta. The encapsulated Fe( Ⅱ )Salen complexes were found to catalyze the cyclohexene oxidation reaction effectually.%采用自由配体法在β沸石的空腔内合成了Fe(Ⅱ)Salen络合物.XRD,SEM,TG-DTA,UV-Vis和元素分析等物理化学方法的分析结果表明,在沸石中的Fe(Ⅱ)Salen是由金属离子与配体以化学计量(摩尔比为1)络合而成,并体现了Fe(Ⅱ)Salen络合物的本征特性.环己烯的催化氧化揭示了β沸石中Fe(Ⅱ)Salen络合物的独特反应性.

  17. Zeólitas hierarquicamente estruturadas Hierarchically structured zeolites

    Directory of Open Access Journals (Sweden)

    Saulo de Tarso Figueiredo Grecco

    2013-01-01

    Full Text Available This review presents the main characteristics and properties of microporous (zeolites and ordered mesoporous materials, focusing on structural aspects and preparation. In addition, their use as heterogeneous catalysts are also discussed, with emphasis on their advantages and disadvantages. Due to difficulty in application of zeolites in the conversion of bulky molecules, the most relevant strategies of synthesis for the preparation of zeolitic materials with hierarchical pore structure was also analyzed, which allow this limitation to be overcome.

  18. Violations of L\\"owensteins rule in zeolites

    OpenAIRE

    Fletcher, Rachel E.; Ling, Sanliang; Slater, Ben

    2016-01-01

    Zeolites, microporous aluminosilicates, are amongst the most widely used catalysts in the petrochemical industry. Zeolite catalytic functionality is coupled to the distribution of tetrahedral alumina (AlO4-) and associated counter-cations throughout the aluminosilicate framework, yet little is definitively known about the factors that govern framework aluminium arrangement. It is generally accepted that all zeolites obey Lowensteins rule of aluminium avoidance and that Al-O-Al linkages are fo...

  19. Selective catalytic conversion of bio-oil over high-silica zeolites.

    Science.gov (United States)

    Widayatno, Wahyu Bambang; Guan, Guoqing; Rizkiana, Jenny; Du, Xiao; Hao, Xiaogang; Zhang, Zhonglin; Abudula, Abuliti

    2015-03-01

    Four high silica zeolites, i.e., HSZ-385, 890, 960, and 990 were utilized for the selective catalytic conversion of bio-oil from Fallopia japonica to certain chemicals in a fixed-bed reactor. The Beta-type HSZ-960 zeolite showed the highest selectivity to hydrocarbons, especially to aromatics as well as PAH compounds with the lowest unwanted chemicals while HSZ-890 showed high selectivity to aromatics. NH3-Temperature Programmed Desorption (TPD) analysis indicated that different amounts of acid sites in different zeolites determined the catalytic activity for the oxygen removal from bio-oil, in which the acid sites at low temperature (LT) region gave more contribution within the utilized temperature region. The reusability test of HSZ-960 showed the stability of hydrocarbons yield at higher temperature due to the significant contribution of coke gasification which assisted further deoxygenation of bio-oil. These results provide a guidance to select suitable zeolite catalysts for the upgrading of bio-oil in a practical process.

  20. Application of novel Polypyrrole/thiol-functionalized zeolite Beta/MCM-41 type mesoporous silica nanocomposite for adsorption of Hg{sup 2+} from aqueous solution and industrial wastewater: Kinetic, isotherm and thermodynamic studies

    Energy Technology Data Exchange (ETDEWEB)

    Javadian, Hamedreza, E-mail: Hamedreza.Javadian@yahoo.com [Department of Chemical Engineering, Shahrood Branch, Islamic Azad University, Shahrood, Islamic Republic of Iran (Iran, Islamic Republic of); Taghavi, Mehdi [Polymer Chemistry Research Laboratory, Department of Chemistry, University of Mazandaran, Babolsar, 47416-95447, Islamic Republic of Iran (Iran, Islamic Republic of)

    2014-01-15

    Hierarchical zeolite consists of both microporous and unordered mesoporous structures. A composite of Polypyrrole/thiol-functionalized Beta/MCM-41 (PPy/SH-Beta/MCM-41) was prepared, characterized by FE-SEM, FT-IR, XRD, TGA and BET analysis and applied in the investigation of its adsorption characteristics for the removal of Hg{sup 2+} ions from aqueous solutions. Thiol-functionalized Beta/MCM-41 (SH-Beta/MCM-41) was prepared by 3-mercaptopropyltrimethoxysilane (MPTMS) in the presence of aerosil-200 as a silica source by two-step hydrothermal crystallization procedure. Batch mode experiments were conducted and three kinetic models were used to describe the adsorption process. The experimental data fitted very well with the Pseudo-second-order kinetic model. The calculated thermodynamic parameters (ΔH, ΔS and ΔG) revealed that the adsorption of Hg{sup 2+} onto PPy/SH-Beta/MCM-41 is an endothermic and spontaneous process. It was found that temperature has a positive effect on the removal efficiency and that PPy/SH-Beta/MCM-41 is potentially able to remove Hg{sup 2+} ions from aqueous solutions at even high concentrations (400 mg L{sup −1}). The recovery of Hg{sup 2+} from the PPy/SH-Beta/MCM-41 adsorbent was found to be more than 90% using 0.5 M H{sub 2}SO{sub 4}, and the ability of the absorbent to be reused for removal of Hg{sup 2+} was investigated.

  1. Zeolite-Y entrapped Ru(III and Fe(III complexes as heterogeneous catalysts for catalytic oxidation of cyclohexane reaction

    Directory of Open Access Journals (Sweden)

    Chetan K. Modi

    2017-02-01

    Full Text Available Catalysis is probably one of the greatest contributions of chemistry to both economic growth and environmental protection. Herein we report the catalytic behavior of zeolite-Y entrapped Ru(III and Fe(III complexes with general formulae [M(VTCH2·2H2O]+-Y and [M(VFCH2·2H2O]+-Y [where, VTCH = vanillin thiophene-2-carboxylic hydrazone and VFCH = vanillin furoic-2-carboxylic hydrazone] over the oxidation of cyclohexane forming cyclohexanone and cyclohexanol. The samples were corroborated by various physico-chemical techniques. These zeolite-Y based complexes are stable and recyclable under current reaction conditions. Amongst them, [Ru(VTCH2⋅2H2O]+-Y showed higher catalytic activity (41.1% with cyclohexanone (84.6% selectivity.

  2. Fluoride-assisted synthesis of bimodal microporous SSZ-13 zeolite

    NARCIS (Netherlands)

    Zhu, Xiaochun; Kosinov, Nikolay; Hofmann, Jan P.; Mezari, Brahim; Qian, Qingyun; Rohling, Roderigh; Weckhuysen, Bert M.; Ruiz-Martinez, Javier; Hensen, Emiel J. M.

    2016-01-01

    The presence of small amount of fluoride in alkaline hydrothermal synthesis of SSZ-13 zeolite yields bimodal microporous particles with substantially improved performance in the methanol-to-olefins (MTO) reaction. Hydrocarbon uptake measurements and fluorescence microspectroscopy of spent catalysts

  3. Zeolites Remove Sulfur From Fuels

    Science.gov (United States)

    Voecks, Gerald E.; Sharma, Pramod K.

    1991-01-01

    Zeolites remove substantial amounts of sulfur compounds from diesel fuel under relatively mild conditions - atmospheric pressure below 300 degrees C. Extracts up to 60 percent of sulfur content of high-sulfur fuel. Applicable to petroleum refineries, natural-gas processors, electric powerplants, and chemical-processing plants. Method simpler and uses considerably lower pressure than current industrial method, hydro-desulfurization. Yields cleaner emissions from combustion of petroleum fuels, and protects catalysts from poisoning by sulfur.

  4. Cr-13 X/K-Cr-13 X分子筛催化剂上二氯甲烷的催化燃烧%Catalytic Combustion of Dichloromethane over Cr-13 X and K-Cr-13 X Zeolites Catalysts

    Institute of Scientific and Technical Information of China (English)

    张丽雷; 刘绍英; 李子健; 姚洁; 王公应

    2014-01-01

    Cr-13 X and K-Cr-13 X zeolites catalysts with different K and Cr contents were prepared by ion ex-change method, and their catalytic performance for catalytic combustion of dichloromethane were evaluated in a conventional fixed bed reactor. Then, these catalysts were characterized via physicochemical techniques. The results showed that, when the Cr content was less than 5.19%, crystallinity of 13X zeolite was not affec-ted by the addition of K and Cr significantly. Cr addition not only enhanced the selectivity of CO2 product, but also eliminated CH3 Cl by-products. The exchange of K with an appropriate amount enhanced the stability and activity of Cr-13X catalyst, as well as the selectivity of CO2 and HCl products. The enhancement of the cata-lytic activity and the products distribution could be accounted for the basis of oxidation and acidity of catalysts. On the condition of gas hourly space velocity of 1í104 h-1 and dichloromethane concentration of 5692 mg/m3 , an optimal 1.31%K-5.01%Cr-13X catalyst was found with t50 at 212 ℃, t98 at 298 ℃ , CO2 selectivity at 60.6% and HCl selectivity at 96.5%, and this catalyst showed relatively stable catalytic activity during 100 h reaction.%以13X分子筛为原料采用离子交换法制备了不同Cr含量的Cr-13X和K-Cr-13X分子筛催化剂,在固定床反应器上研究了催化剂对二氯甲烷的催化燃烧性能.研究结果表明, Cr含量(质量分数)小于5.19%时,对催化剂的结构没有明显影响.添加Cr提高了CO2的选择性,无CH3 Cl副产物生成.交换适量的K可以提高Cr-13X催化剂的活性和稳定性,并提高CO2和HCl的选择性.催化剂的表面酸性和氧化性是影响催化剂活性和产物分布的主要因素.在空速为1×104 h-1,二氯甲烷浓度为5692 mg/m3的条件下,1.31%K-5.01%Cr-13X分子筛催化剂对二氯甲烷催化燃烧50%的温度( t50)为212℃,燃烧98%的温度( t98)为298℃, CO2选择性为60.6%, HCl选择性为96.5%,连续反应100 h,未发现有明显失活现象.

  5. UTILITY OF SYNTHETIC ZEOLITES IN REMOVAL OF INORGANIC AND ORGANIC WATER POLLUTANTS

    Science.gov (United States)

    Zeolites are well known for their ion exchange and adsorption properties. Different inorganic and organic pollutants have been removed from water at room temperature using various zeolites. Synthetic zeolites like ZSM-5, Ferrierite, Beta and Faujasite Y have been used to remove i...

  6. Zeolite-catalyzed biomass conversion to fuels and chemicals

    DEFF Research Database (Denmark)

    Taarning, Esben; Osmundsen, Christian Mårup; Yang, Xiaobo

    2011-01-01

    Heterogeneous catalysts have been a central element in the efficient conversion of fossil resources to fuels and chemicals, but their role in biomass utilization is more ambiguous. Zeolites constitute a promising class of heterogeneous catalysts and developments in recent years have demonstrated...... their potential to find broad use in the conversion of biomass. In this perspective we review and discuss the developments that have taken place in the field of biomass conversion using zeolites. Emphasis is put on the conversion of lignocellulosic material to fuels using conventional zeolites as well...

  7. Congressionally Directed Project for Passive NOx Removal Catalysts Research

    Energy Technology Data Exchange (ETDEWEB)

    Schneider, William

    2014-08-29

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

  8. Congressionally Directed Project for Passive NOx Removal Catalysts Research

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-12-29

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

  9. Zeolite-catalyzed isomerization of tetroses in aqueous medium

    DEFF Research Database (Denmark)

    Shunmugavel, Saravanamurugan; Riisager, Anders

    2014-01-01

    The isomerization of erythrose (ERO) was studied in water over commercially available large-pore zeolites such as, e.g. H-Y, H-USY and H-beta. Among the employed zeolites, H-USY(6) was found to efficiently isomerize the sugar yielding 45 % erythrulose (ERU), 42 % ERO and 3 % of the epimer threose...

  10. A novel urea conductometric biosensor based on zeolite immobilized urease.

    Science.gov (United States)

    Kirdeciler, Salih Kaan; Soy, Esin; Oztürk, Seçkin; Kucherenko, Ivan; Soldatkin, Oleksandr; Dzyadevych, Sergei; Akata, Burcu

    2011-09-15

    A new approach was developed for urea determination where a thin film of silicalite and zeolite Beta deposited onto gold electrodes of a conductometric biosensor was used to immobilize the enzyme. Biosensor responses, operational and storage stabilities were compared with results obtained from the standard membrane methods for the same measurements. For this purpose, different surface modification techniques, which are simply named as Zeolite Membrane Transducers (ZMTs) and Zeolite Coated Transducers (ZCTs) were compared with Standard Membrane Transducers (SMTs). Silicalite and zeolite Beta with Si/Al ratios 40, 50 and 60 were used to modify the conductometric electrodes and to study the biosensor responses as a function of changing zeolitic parameters. During the measurements using ZCT electrodes, there was no need for any cross-linker to immobilize urease, which allowed the direct evaluation of the effect of changing Si/Al ratio for the same type of zeolite on the biosensor responses for the first time. It was seen that silicalite and zeolite Beta added electrodes in all cases lead to increased responses with respect to SMTs. The responses obtained from ZCTs were always higher than ZMTs as well. The responses obtained from zeolite Beta modified ZMTs and ZCTs increased as a function of increasing Si/Al ratio, which might be due to the increased hydrophobicity and/or the acid strength of the medium.

  11. Structures and reaction mechanisms of cumene formation via benzene alkylation with propylene in a newly synthesized ITQ-24 zeolite: an embedded ONIOM study.

    Science.gov (United States)

    Jansang, Bavornpon; Nanok, Tanin; Limtrakul, Jumras

    2006-06-29

    The cumene formation via benzene alkylation with propylene on the new three-dimensional nanoporous catalyst, ITQ-24 zeolite, has been investigated by using the ONIOM2(B3LYP/6-31G(d,p):UFF) method. Both consecutive and associative reaction pathways are examined. The contributions of the short-range van der Waals interactions, which are explicitly included in the ONIOM2 model, and an additional long-range electrostatic potential from the extended zeolite framework to the energy profile are taken into consideration. It is found that benzene alkylation with propylene in the ITQ-24 zeolite prefers to occur through the consecutive reaction mechanism. The benzene alkylation step is the reaction rate-determining step with an estimated activation energy of 35.70 kcal/mol, comparable with an experimental report in beta-zeolite of 34.9 kcal/mol. The electrostatic potential from the extended zeolite framework shows a much more significant contribution to the transition state selectivity than the van der Waals interactions.

  12. Synthesis and characterization of Sn/zeolite and catalytic activity test in the esterification reaction of sludge oil

    Science.gov (United States)

    Alimuddin, Andi Hairil; Usman, Thamrin; Wahyuni, Nelly; Rudiyansyah, Prawatya, Yopa Eka; Astar, Ismail; Yustira, Yudi

    2017-03-01

    Synthesis of Sn-Zeolite has been made to use for esterification reaction of free fatty acids in sludge oil. Catalyst characterization was accomplished using X-Ray Diffraction (XRD), X-Ray Flourecence (XRF), and Fourier Transform Infra Red (FTIR). Catalyst Sn/zeolite was synthesized by impregnated Sn of SnCl2 into the zeolite. The amount of Sn impregnated base on the value of cation exchange capacity (CEC) of zeolites. Esterification reaction of fatty acids from sludge oil using Sn/Zeolite catalyst was did by variated the reaction time. XRD analysis results showed that the catalyst Sn/zeolite was dominated by modernit and quartz. XRF analysis results was increasing amount of Sn metal and the Si/Al ratio on Sn/zeolite catalyst along with addition of Sn metal. FTIR analysis results showed that the catalyst synthesized had Bronsted acid side (the spectrum 1639.4; 1656.7; 1654.8 cm-1) and the Lewis acid (spectrum 1400.2 and 1402.2 cm-1). The results showed that the optimum conditions of esterification reaction in 4 hours reaction time, 5% concentration of the catalyst, and molar ratio was about 1:10 with a conversion percentage of products reached 96.00%, which can be achieved with a ratio was about 4:1 between Sn and zeolite on Sn/zeolite catalyst.

  13. [Zeolite catalysis in conversion of cellulosics

    Energy Technology Data Exchange (ETDEWEB)

    Tsao, G.T.

    1992-01-01

    To transform biomass into fermentable substrate for yeast, we are using zeolites instead of enzymes to catalyze the two bottleneck reactions in biomass conversion, xylose isomerization and ceuobiose hydrolysis. The experimental results on these reactions carried out over various zeolites and other catalysts are presented herein. The advantages and disadvantages of using these catalysts over enzymes are also discussed. Heterogeneous solid catalysts other than zeolites has been employed for cellobiose-to-glucose hydrolysis. The size and shape selectivity that makes zeoutes unique for some reactions can add diffusional hindrance. We have spent some time screening various known solid acidic catalysts. We report that a class of cationic ion exchange resins in the acidified form (e.g. Amberlite) has worked well as an acidic catalyst in hydrolyzing cellobiose to glucose. Our experimental results, together with those obtained from a homogeneous acid catalyst (e.g. sulfuric acid) for comparison are provided. Having succeeded in finding an alternative solid acid catalyst for hydrolysis, we explored other solid resin or other homogeneous but non-enzyme catalyst to carry out the xylose-to-xylulose isomerization. A fairly extensive search has been made. We explored the use of sodium aluminates in the homogeneous phase isomerization of glucose to fructose and obtained a very high conversion of glucose to fructose with the final mixture containing 85% of fructose instead of the common 45%. Fructose apparently complexes with aluminates, and its equilibrium concentration is shifted to considerably higher values than permitted by simple glucose/fructose equilibrium. We have recently found a number of catalysts capable of promoting isomerization between aldoses and ketoses. One solid resin, known as polyvinyl pyridine (PVP), is able to convert xylose to xylulose at a pH below 7. Our usage of alternative isomerization catalysts, including PVP, are described.

  14. [Zeolite catalysis in conversion of cellulosics

    Energy Technology Data Exchange (ETDEWEB)

    Tsao, G.T.

    1992-12-31

    To transform biomass into fermentable substrate for yeast, we are using zeolites instead of enzymes to catalyze the two bottleneck reactions in biomass conversion, xylose isomerization and ceuobiose hydrolysis. The experimental results on these reactions carried out over various zeolites and other catalysts are presented herein. The advantages and disadvantages of using these catalysts over enzymes are also discussed. Heterogeneous solid catalysts other than zeolites has been employed for cellobiose-to-glucose hydrolysis. The size and shape selectivity that makes zeoutes unique for some reactions can add diffusional hindrance. We have spent some time screening various known solid acidic catalysts. We report that a class of cationic ion exchange resins in the acidified form (e.g. Amberlite) has worked well as an acidic catalyst in hydrolyzing cellobiose to glucose. Our experimental results, together with those obtained from a homogeneous acid catalyst (e.g. sulfuric acid) for comparison are provided. Having succeeded in finding an alternative solid acid catalyst for hydrolysis, we explored other solid resin or other homogeneous but non-enzyme catalyst to carry out the xylose-to-xylulose isomerization. A fairly extensive search has been made. We explored the use of sodium aluminates in the homogeneous phase isomerization of glucose to fructose and obtained a very high conversion of glucose to fructose with the final mixture containing 85% of fructose instead of the common 45%. Fructose apparently complexes with aluminates, and its equilibrium concentration is shifted to considerably higher values than permitted by simple glucose/fructose equilibrium. We have recently found a number of catalysts capable of promoting isomerization between aldoses and ketoses. One solid resin, known as polyvinyl pyridine (PVP), is able to convert xylose to xylulose at a pH below 7. Our usage of alternative isomerization catalysts, including PVP, are described.

  15. Effect of vanadium on the deactivation of FCC catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Roncolatto, R.E.; Lam, Y.L. [PETROBRAS, Rio de Janeiro, RJ (Brazil). Centro de Pesquisas. Div. de Catalisadores]. E-mail: roncolatto@cenpes.petrobras.com.br; y12@cenpes.petrobras.com.br

    1998-06-01

    This work provides concrete evidence that causes the destruction of the zeolite in the FCC catalysts by a mechanism of acid attack or solid-solid transformation, as well as additional dealumination of the zeolite framework in the presence of steam and at high temperature. While these effects resulted in the reduction in crystallinity (zeolite Y content), specific area and unit cell size of the Y zeolite as the amount of vanadium in the catalysts increased, the reduction in activity was the most pronounced. The differences in these behaviors were interpreted and the model can be used for better catalyst formulation or screening. (author)

  16. EFFECT OF VANADIUM ON THE DEACTIVATION OF FCC CATALYSTS

    Directory of Open Access Journals (Sweden)

    Roncolatto R.E

    1998-01-01

    Full Text Available This work provides concrete evidence that vanadium causes the destruction of the zeolite in the FCC catalysts by a mechanism of acid attack or solid-solid transformation, as well as additional dealumination of the zeolite framework in the presence of steam and at high temperature. While these effects resulted in the reduction in crystallinity (zeolite Y content, specific area and unit cell size of the Y zeolite as the amount of vanadium in the catalysts increased, the reduction in activity was the most pronounced. The differences in these behaviors were interpreted and the model can be used for better catalyst formulation or screening.

  17. Experimental research of pulsed discharge plasma and TiO2/Zeolite coupling technology for formaldehyde removal

    Science.gov (United States)

    Dong, Bingyan; Lan, Shuirong

    2013-03-01

    The pulsed discharge plasma combining with catalyst to remove formaldehyde is a novel type of advanced oxidation technology. In the present work, taking wire-tube pulsed discharge plasma and TiO2/Zeolite coupling technology for formaldehyde removal. The studies have investigated the wire-tube reactor with zeolite, TiO2, TiO2/Zeolite for formaldehyde removal respectively. Results show that in the optimal experimental conditions and the baking time is 120 min, the baking temperature is 450 °C, that TiO2/Zeolite catalyst which made by sol-gel shows higher photocatalytic activity and efficiency. The pulsed discharge with TiO2/Zeolite catalyst for formaldehyde removal has higher removal efficiency than pulsed discharge with zeolite or TiO2. Therefore, pulsed discharge plasma with TiO2/Zeolite for the removal of formaldehyde can greatly increase the removal efficiency.

  18. Current Understanding of Cu-Exchanged Chabazite Molecular Sieves for Use as Commercial Diesel Engine DeNOx Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Gao, Feng; Kwak, Ja Hun; Szanyi, Janos; Peden, Charles HF

    2013-11-03

    Selective catalytic reduction (SCR) of NOx with ammonia using metal-exchanged molecular sieves with a chabazite (CHA) structure has recently been commercialized on diesel vehicles. One of the commercialized catalysts, i.e., Cu-SSZ-13, has received much attention for both practical and fundamental studies. For the latter, the particularly well-defined structure of this zeolite is allowing long-standing issues of the catalytically active site for SCR in metal-exchanged zeolites to be addressed. In this review, recent progress is summarized with a focus on two areas. First, the technical significance of Cu-SSZ-13 as compared to other Cu-ion exchanged zeolites (e.g., Cu-ZSM-5 and Cu-beta) is highlighted. Specifically, the much enhanced hydrothermal stability for Cu-SSZ-13 compared to other zeolite catalysts is addressed via performance measurements and catalyst characterization using several techniques. The enhanced stability of Cu-SSZ-13 is rationalized in terms of the unique small pore structure of this zeolite catalyst. Second, the fundamentals of the catalytically active center; i.e., the chemical nature and locations within the SSZ-13 framework are presented with an emphasis on understanding structure-function relationships. For the SCR reaction, traditional kinetic studies are complicated by intra-particle diffusion limitations. However, a major side reaction, nonselective ammonia oxidation by oxygen, does not suffer from mass-transfer limitations at relatively low temperatures due to significantly lower reaction rates. This allows structure-function relationships that are rather well understood in terms of Cu ion locations and redox properties. Finally, some aspects of the SCR reaction mechanism are addressed on the basis of in-situ spectroscopic studies.

  19. Highly dispersed iron species created on alkali-treated zeolite for ammonia SCR

    Institute of Scientific and Technical Information of China (English)

    Jing Ma; Duan Weng; Xiaodong Wu; Zhichun Si; Zhenwei Wu

    2013-01-01

    Alkaline treatment using sodium hydroxide was introduced to obtain a hierarchical pore structure in H-ZSM-5 zeolite. Fe-exchanged zeolite catalysts were prepared by impregnation on the original and alkali-treated zeolites, and were evaluated for NOx reduction by NH3, NO oxidation, and NH3 oxidation reactions. The highly dispersed iron species as active sites can be obtained by controlling the pore structure and particle size of zeolite. Therefore, the Fe/ZSM-5 catalyst treated mildly by sodium hydroxide before iron exchange, which contains amounts of highly dispersed Fe species, obtains over 80% NOx conversion at a wide temperature range of 250-500 1C.

  20. Templating mesoporous zeolites

    DEFF Research Database (Denmark)

    Egeblad, Kresten; Christensen, Christina Hviid; Kustova, Marina

    2008-01-01

    The application of templating methods to produce zeolite materials with hierarchical bi- or trimodal pore size distributions is reviewed with emphasis on mesoporous materials. Hierarchical zeolite materials are categorized into three distinctly different types of materials: hierarchical zeolite...... crystals, nanosized zeolite crystals, and supported zeolite crystals. For the pure zeolite materials in the first two categories, the additional meso- or macroporosity can be classified as being either intracrystalline or intercrystalline, whereas for supported zeolite materials, the additional porosity...... originates almost exclusively from the support material. The methods for introducing mesopores into zeolite materials are discussed and categorized. In general, mesopores can be templated in zeolite materials by use of solid templating, supramolecular templating, or indirect templating...

  1. Hydrophobic Fe-zeolites for removal of MTBE from water by combination of adsorption and oxidation.

    Science.gov (United States)

    Gonzalez-Olmos, Rafael; Kopinke, Frank-Dieter; Mackenzie, Katrin; Georgi, Anett

    2013-03-05

    Several zeolites were evaluated as adsorbents for the removal of MTBE from water in a screening process. It was observed that the SiO2/Al2O3 molar ratio is a decisive factor for the adsorption properties, at least in the case of ZSM5 zeolites. ZSM5 zeolites with SiO2/Al2O3 ratios >200 were found to provide the best sorption properties for MTBE. To design a combined sorption/reaction method, regeneration of the loaded zeolites by selected advanced oxidation processes (AOP) was studied: (1) Fenton treatment using H2O2 with dissolved iron salts and (2) heterogeneous Fenton-like oxidation with Fe immobilized on the zeolites. The first was ineffective in regenerating loaded zeolites. However, heterogeneous catalysis using Fe species immobilized on the zeolite by liquid ion exchange was markedly more effective. Although these hydrophobic zeolites have a low ion exchange capacity, resulting in iron loadings of ≤ 0.09 wt %, it was possible to obtain sufficiently active catalysts. Hydrophobic Fe-zeolites can therefore be regarded as promising materials for the removal of MTBE from water, since they allow the combination of efficient adsorption and oxidative degradation of MTBE by H2O2. In contrast to the homogeneous catalysis by dissolved iron ions, these heterogeneous catalysts work at near-neutral pH and can be easily reused. Fe-zeolites as adsorbents/catalysts showed a good stability in both batch and column experiments.

  2. Beyond Creation of Mesoporosity: The Advantages of Polymer-Based Dual-Function Templates for Fabricating Hierarchical Zeolites

    KAUST Repository

    Tian, Qiwei

    2016-02-05

    Direct synthesis of hierarchical zeolites currently relies on the use of surfactant-based templates to produce mesoporosity by the random stacking of 2D zeolite sheets or the agglomeration of tiny zeolite grains. The benefits of using nonsurfactant polymers as dual-function templates in the fabrication of hierarchical zeolites are demonstrated. First, the minimal intermolecular interactions of nonsurfactant polymers impose little interference on the crystallization of zeolites, favoring the formation of 3D continuous zeolite frameworks with a long-range order. Second, the mutual interpenetration of the polymer and the zeolite networks renders disordered but highly interconnected mesopores in zeolite crystals. These two factors allow for the synthesis of single-crystalline, mesoporous zeolites of varied compositions and framework types. A representative example, hierarchial aluminosilicate (meso-ZSM-5), has been carefully characterized. It has a unique branched fibrous structure, and far outperforms bulk aluminosilicate (ZSM-5) as a catalyst in two model reactions: conversion of methanol to aromatics and catalytic cracking of canola oil. Third, extra functional groups in the polymer template can be utilized to incorporate desired functionalities into hierarchical zeolites. Last and most importantly, polymer-based templates permit heterogeneous nucleation and growth of mesoporous zeolites on existing surfaces, forming a continuous zeolitic layer. In a proof-of-concept experiment, unprecedented core-shell-structured hierarchical zeolites are synthesized by coating mesoporous zeolites on the surfaces of bulk zeolites. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Development of GREET Catalyst Module

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Zhichao [Argonne National Lab. (ANL), Argonne, IL (United States); Benavides, Pahola T. [Argonne National Lab. (ANL), Argonne, IL (United States); Dunn, Jennifer B. [Argonne National Lab. (ANL), Argonne, IL (United States); Cronauer, Donald C. [Argonne National Lab. (ANL), Argonne, IL (United States)

    2015-09-01

    In this report, we develop energy and material flows for the production of five different catalysts (tar reforming, alcohol synthesis, Zeolite Socony Mobil-5 [ZSM-5], Mo/Co/ γ-Al2O3, and Pt/ γ-Al2O3) and two chemicals (olivine, dimethyl ether of polyethylene glycol [DEPG]). These compounds and catalysts are now included in the Greenhouse Gases, Regulated Emissions and Energy Use in Transportation (GREET™) catalyst module.

  4. Catalysts and process for liquid hydrocarbon fuel production

    Science.gov (United States)

    White, Mark G; Liu, Shetian

    2014-12-09

    The present invention provides a novel process and system in which a mixture of carbon monoxide and hydrogen synthesis gas, or syngas, is converted into hydrocarbon mixtures composed of high quality gasoline components, aromatic compounds, and lower molecular weight gaseous olefins in one reactor or step. The invention utilizes a novel molybdenum-zeolite catalyst in high pressure hydrogen for conversion, as well as a novel rhenium-zeolite catalyst in place of the molybdenum-zeolite catalyst, and provides for use of the novel catalysts in the process and system of the invention.

  5. REY-zeolite and silica-alumina mixed support for hydrotreating heavy gas oil

    Energy Technology Data Exchange (ETDEWEB)

    Sambi, I.S.; Mann, R.S. (Univ. of Ottawa, Ottawa, ON (Canada))

    1989-04-01

    Rare earth exchanged Y-type zeolite (REY-zeolite) was dispersed in a silica-alumina gel to prepare catalyst supports with better hydrogenolysis activity. Such support material showed improved hydrotreating properties compared to commercial catalysts, expecially for heavy gas oils. Statistical experimental designs used to optimize the composition of such mixed supports suggested a composition of 10 wt.% silica, 25 wt.% zeolite and 65 wt.% alumina as optimum for hydrotreating a heavy gas oil (343{sup 0}C to 525{sup 0}C fraction) obtained from hydrocracking of Athabasca bitumen. The kinetic parameters were then evolved for teh optimum catalyst. 6 refs., 7 figs., 10 tabs.

  6. Effect of ammonia on catalytic properties of an AShNTs-3 catalyst containing zeolite in alkylation of phenols with styrene

    Energy Technology Data Exchange (ETDEWEB)

    Kolesnichenko, N.V. (A.V. Topchiyev Inst. of Petrochemical Synthesis, USSR); Kurashev, M.V.; Romanovskii, B.V.; Menyailov, A.A.

    1981-01-01

    A study was made of the effect of previous treatment with an ammonia mixture with a small proportion of steam on catalytic properties of AShNTs-3. Preliminary treatment of the catalyst with a mixture of ammonia and steam at 250/sup 0/C for 2 hr increases considerably the yield of methylbenzylphenols, particularly 2-(..cap alpha..-methylbenzyl)phenol. Highest yield of methylbenzylphenols is achieved at a temperature of 250/sup 0/C, a molar ratio of phenol : styrene of 4 : 1 and a space velocity of 5.5 hr/sup -1/.

  7. Biosensors Based on Nano-Gold/Zeolite-Modified Ion Selective Field-Effect Transistors for Creatinine Detection

    Science.gov (United States)

    Ozansoy Kasap, Berna; Marchenko, Svitlana V.; Soldatkin, Oleksandr O.; Dzyadevych, Sergei V.; Akata Kurc, Burcu

    2017-03-01

    The combination of advantages of using zeolites and gold nanoparticles were aimed to be used for the first time to improve the characteristic properties of ion selective field-effect transistor (ISFET)-based creatinine biosensors. The biosensors with covalently cross-linked creatinine deiminase using glutaraldehyde (GA) were used as a control group, and the effect of different types of zeolites on biosensor responses was investigated in detail by using silicalite, zeolite beta (BEA), nano-sized zeolite beta (Nano BEA) and zeolite BEA including gold nanoparticle (BEA-Gold). The presence of gold nanoparticles was investigated by ICP, STEM-EDX and XPS analysis. The chosen zeolite types allowed investigating the effect of aluminium in the zeolite framework, particle size and the presence of gold nanoparticles in the zeolitic framework.

  8. Synthesis and catalytic applications of combined zeolitic/mesoporous materials

    Directory of Open Access Journals (Sweden)

    Jarian Vernimmen

    2011-11-01

    Full Text Available In the last decade, research concerning nanoporous siliceous materials has been focused on mesoporous materials with intrinsic zeolitic features. These materials are thought to be superior, because they are able to combine (i the enhanced diffusion and accessibility for larger molecules and viscous fluids typical of mesoporous materials with (ii the remarkable stability, catalytic activity and selectivity of zeolites. This review gives an overview of the state of the art concerning combined zeolitic/mesoporous materials. Focus is put on the synthesis and the applications of the combined zeolitic/mesoporous materials. The different synthesis approaches and formation mechanisms leading to these materials are comprehensively discussed and compared. Moreover, Ti-containing nanoporous materials as redox catalysts are discussed to illustrate a potential implementation of combined zeolitic/mesoporous materials.

  9. Synthesis strategies in the search for hierarchical zeolites.

    Science.gov (United States)

    Serrano, D P; Escola, J M; Pizarro, P

    2013-05-07

    formation of organic-inorganic composites that, upon calcination, are transformed into hierarchical zeolites. However, in spite of this impressive progress in novel strategies for the preparation of hierarchical zeolites, significant challenges are still ahead. The overall one is the development of methods that are versatile in terms of zeolite structures and compositions, capable of tuning the secondary porosity properties, and being scaled up in a cost-effective way. Recent works have demonstrated that it is possible to scale-up easily the synthesis of hierarchical zeolites by desilication. Economic aspects may become a significant bottleneck for the commercial application of hierarchical zeolites since most of the synthesis strategies so far developed imply the use of more expensive procedures and reagents compared to conventional zeolites. Nevertheless, the use of hierarchical zeolites as efficient catalysts for the production of high value-added compounds could greatly compensate these increased manufacturing costs.

  10. First Principles Simulations of Hydrocarbon Conversion Processes in Functionalized Zeolitic Materials

    Science.gov (United States)

    Mazar, Mark Nickolaus

    is responsible for the largest activation energy of the catalytic cycle. This assessment is similar to the findings of alkane metathesis studies on alumina/silica supports and indicates that the entire AM cycle can be performed in zeolites by isolated single-atom transition metal hydrides. Performed over acid form zeolites, MTH is used in the conversion of methanol into a broad range of hydrocarbons, including alkenes, alkanes, and aromatics. For reasons that are not yet rigorously quantified, product selectivities vary dramatically based on the choice of catalyst and reaction conditions. The methylation of species containing double bonds (i.e., co-catalysts) is central to the overall process. Distinct structure-function relationships were found with respect to the elementary steps in the methylation and beta-scission of olefins. In Chapter 4, the role of zeolite topology in the step-wise methylation of ethene by surface methoxides is investigated. Elementary steps are studied across multiple frameworks (i.e., BEA, CHA, FER, MFI, and MOR) constituting a wide variety of confinement environments. The reaction of surface methoxides with ethene is found to require a transition state containing a primary carbocation. The barrier height is found to decrease nearly monotonically with respect to the degree of dispersion interactions stabilizing the primary carbocationic species in the transition state. In addition, quantification of the ``local'' dispersion energy indicates that confinement effects can not be simply correlated to pore size. The beta-scission of olefins plays an important role in the product selectivities of many important chemical processes, including MTH. In Chapter 5, beta-scission modes involving C6 and C8 isomers are investigated at a single, isolated Bronsted acid site within H-ZSM-5. We find that the relative enthalpic barriers of beta-scission elementary steps can be rationalized by the substitution order of the two different carbocationic carbon

  11. Effects of preparation variables of supported-cobalt catalysts on the selective hydrogenation of. alpha. ,. beta. -unsaturated aldehydes

    Energy Technology Data Exchange (ETDEWEB)

    Nitta, Yuriko; Hiramatsu, Yoshifumi; Imanaka, Toshinobu (Osaka Univ., Toyonaka (Japan))

    1990-11-01

    The effects of starting salts, supports, added amount of Na{sub 2}CO{sub 3}, and other precipitation variables on catalytic properties of supported cobalt catalysts were studied for the hydrogenation of cinnamaldehyde and crotonaldehyde by using TGA, XRD, and XPS. The catalysts prepared from cobalt chloride always exhibited high selectivities to unsaturated alcohols irrespective of the support employed. The amount of surface chlorine remaining after H{sub 2}-reduction of the Co/SiO{sub 2} precursors prepared from cobalt chloride decreased with increasing amount of Na{sub 2}CO{sub 3} added as the precipitant, and both activity and selectivity reached maxima at around Cl/Co = 0.2 in the catalyst surface. The enhanced selectivity of the catalyst prepared from cobalt chloride was explained by the effects of residual chlorine both in the H{sub 2}-reduction stage and in the reaction stage; the former leads to a favorable crystallite size distribution (CDS) of cobalt and the latter depresses the hydrogenation of C{double bond}C double bond. The difference in activities and selectivities of various supported catalysts prepared from cobalt nitrate was discussed based on the difference in the strength of metal-support interaction which leads to different CDSs of cobalt in theses catalysts.

  12. Zeolite Crystal Growth (ZCG) Flight on USML-2

    Science.gov (United States)

    Sacco, Albert, Jr.; Bac, Nurcan; Warzywoda, Juliusz; Guray, Ipek; Marceau, Michelle; Sacco, Teran L.; Whalen, Leah M.

    1997-01-01

    The extensive use of zeolites and their impact on the world's economy has resulted in many efforts to characterize their structure, and improve the knowledge base for nucleation and growth of these crystals. The zeolite crystal growth (ZCG) experiment on USML-2 aimed to enhance the understanding of nucleation and growth of zeolite crystals, while attempting to provide a means of controlling the defect concentration in microgravity. Zeolites A, X, Beta, and Silicalite were grown during the 16 day - USML-2 mission. The solutions where the nucleation event was controlled yielded larger and more uniform crystals of better morphology and purity than their terrestrial/control counterparts. The external surfaces of zeolite A, X, and Silicalite crystals grown in microgravity were smoother (lower surface roughness) than their terrestrial controls. Catalytic studies with zeolite Beta indicate that crystals grown in space exhibit a lower number of Lewis acid sites located in micropores. This suggests fewer structural defects for crystals grown in microgravity. Transmission electron micrographs (TEM) of zeolite Beta crystals also show that crystals grown in microgravity were free of line defects while terrestrial/controls had substantial defects.

  13. Reliable method for the synthesis of aryl beta-D-glucopyranosides, using boron trifluoride-diethyl ether as catalyst

    NARCIS (Netherlands)

    Smits, E; Engberts, JBFN; Kellogg, RM; vanDoren, HA

    1996-01-01

    Stereospecific formation of aryl 2,3,4,6-tetra-O-acetyl-beta-D-glucopyranoside was achieved by reaction of penta-O-aceeyl-beta-D-glucose 1 with substituted phenols in the presence of boron trifluoride. Yields of the purified products varied from 52-85%. Benzyl alcohol could also be glucosylated usin

  14. Towards a sustainable manufacture of hierarchical zeolites.

    Science.gov (United States)

    Verboekend, Danny; Pérez-Ramírez, Javier

    2014-03-01

    Hierarchical zeolites have been established as a superior type of aluminosilicate catalysts compared to their conventional (purely microporous) counterparts. An impressive array of bottom-up and top-down approaches has been developed during the last decade to design and subsequently exploit these exciting materials catalytically. However, the sustainability of the developed synthetic methods has rarely been addressed. This paper highlights important criteria to ensure the ecological and economic viability of the manufacture of hierarchical zeolites. Moreover, by using base leaching as a promising case study, we verify a variety of approaches to increase reactor productivity, recycle waste streams, prevent the combustion of organic compounds, and minimize separation efforts. By reducing their synthetic footprint, hierarchical zeolites are positioned as an integral part of sustainable chemistry.

  15. Aluminum-rich mesoporous MFI - type zeolite single crystals

    DEFF Research Database (Denmark)

    Kustova, Marina; Kustov, Arkadii; Christensen, Christina Hviid

    2005-01-01

    Zeolitcs are crystalline materials, which are widely used as solid acid catalysts and supports in many industrial processes. Recently, mesoporous MFI-type zeolite single crystals were synthesized by use of carbon particles as a mesopore template and sodium aluminate as the aluminum Source...... are characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), ammonia temperature programmed desorption (NH3-TPD), and N-2 adsorption measurements. The obtained zeolites combine the high crystallinity and the characteristic micropores of zeolites with an intracrystalline mesopore system...

  16. Synthesis and characterization of Fe(III)-piperazine-derived complexes encapsulated in zeolite Y

    Energy Technology Data Exchange (ETDEWEB)

    Berezuk, Marcio E., E-mail: berezuk@utfpr.edu.br [Universidade Tecnologica Federal do Parana (UTFPR), Apucarana, PR (Brazil); Paesano Junior, Andrea [Dept. de Fisica, Universidade Estadual de Maringa, Maringa, (Brazil); Carvalho, Nakedia M.F. [Departament of Chemistry, Massachusetts Institute of Technology, Cambridge, MA (United States); Horn Junior, Adolfo; Arroyo, Pedro A. [Laboratorio de Ciencias Quimicas, Universidade Estadual do Norte Fluminense (UENF), Campos dos Goytacazes, RJ (Brazil); Cardozo-Filho, Lucio [Dept. de Engenharia Quimica, Universidade Estadual de Maringa, PR (Brazil)

    2012-07-01

    Zeolite-encapsulated complexes have been widely applied in hydrocarbon oxidation catalysis. The 'ship-in-a-bottle' encapsulation of iron(III) complexes containing piperazine and piperazine-derivative ligands in zeolite-Y is described. The flexible ligand methodology was employed and the efficiency and reproducibility of the procedure was investigated. The catalysts were characterized employing several techniques and the results indicate the presence of coordinated and uncoordinated iron(III) ions inside and outside the zeolitic cage. (author)

  17. Tailoring ZSM-5 Zeolites for the Fast Pyrolysis of Biomass to Aromatic Hydrocarbons

    DEFF Research Database (Denmark)

    Hoff, Thomas C.; Gardner, David W.; Thilakaratne, Rajeeva

    2016-01-01

    The production of aromatic hydrocarbons from cellulose by zeolite-catalyzed fast pyrolysis involves a complex reaction network sensitive to the zeolite structure, crystallinity, elemental composition, porosity, and acidity. The interplay of these parameters under the reaction conditions represents...... a major roadblock that has hampered significant improvement in catalyst design for over a decade. Here, we studied commercial and laboratory-synthesized ZSM-5 zeolites and combined data from 10 complementary characterization techniques in an attempt to identify parameters common to high...

  18. Synthesis and characterization of Fe(III-piperazine-derived complexes encapsulated in zeolite Y

    Directory of Open Access Journals (Sweden)

    Márcio E. Berezuk

    2012-01-01

    Full Text Available Zeolite-encapsulated complexes have been widely applied in hydrocarbon oxidation catalysis. The "ship-in-a-bottle" encapsulation of iron(III complexes containing piperazine and piperazine-derivative ligands in zeolite-Y is described. The flexible ligand methodology was employed and the efficiency and reproducibility of the procedure was investigated. The catalysts were characterized employing several techniques and the results indicate the presence of coordinated and uncoordinated iron(III ions inside and outside the zeolitic cage.

  19. Distribution of metal and adsorbed guest species in zeolites

    Energy Technology Data Exchange (ETDEWEB)

    Chmelka, B.F.

    1989-12-01

    Because of their high internal surface areas and molecular-size cavity dimensions, zeolites are used widely as catalysts, shape- selective supports, or adsorbents in a variety of important chemical processes. For metal-catalyzed reactions, active metal species must be dispersed to sites within the zeolite pores that are accessible to diffusing reactant molecules. The distribution of the metal, together with transport and adsorption of reactant molecules in zeolite powders, are crucial to ultimate catalyst performance. The nature of the metal or adsorbed guest distribution is known, however, to be dramatically dependent upon preparatory conditions. Our objective is to understand, at the molecular level, how preparatory treatments influence the distribution of guest species in zeolites, in order that macroscopic adsorption and reaction properties of these materials may be better understood. The sensitivity of xenon to its adsorption environment makes {sup 129}Xe NMR spectroscopy an important diagnostic probe of metal clustering and adsorbate distribution processes in zeolites. The utility of {sup 129}Xe NMR depends on the mobility of the xenon atoms within the zeolite-guest system, together with the length scale of the sample heterogeneity being studied. In large pore zeolites containing dispersed guest species, such as Pt--NaY, {sup 129}Xe NMR is insensitive to fine structural details at room temperature.

  20. Tracing catalytic conversion on single zeolite crystals in 3D with nonlinear spectromicroscopy

    NARCIS (Netherlands)

    Domke, K.F.; Riemer, T.A.; Rago, G.; Parvulescu, A.N.; Bruijnincx, P.C.A.; Enejder, A.; Weckhuysen, B.M.; Bonn, M.

    2012-01-01

    The cost- and material-efficient development of nextgeneration catalysts would benefit greatly from a molecular-level understanding of the interaction between reagents and catalysts in chemical conversion processes. Here, we trace the conversion of alkene and glycol in single zeolite catalyst partic

  1. Design of Ru-zeolites for hydrogen-free production of conjugated linoleic acids.

    Science.gov (United States)

    Philippaerts, An; Goossens, Steven; Vermandel, Walter; Tromp, Moniek; Turner, Stuart; Geboers, Jan; Van Tendeloo, Gustaaf; Jacobs, Pierre A; Sels, Bert F

    2011-06-20

    While conjugated vegetable oils are currently used as additives in the drying agents of oils and paints, they are also attractive molecules for making bio-plastics. Moreover, conjugated oils will soon be accepted as nutritional additives for "functional food" products. While current manufacture of conjugated vegetable oils or conjugated linoleic acids (CLAs) uses a homogeneous base as isomerisation catalyst, a heterogeneous alternative is not available today. This contribution presents the direct production of CLAs over Ru supported on different zeolites, varying in topology (ZSM-5, BETA, Y), Si/Al ratio and countercation (H(+), Na(+), Cs(+)). Ru/Cs-USY, with a Si/Al ratio of 40, was identified as the most active and selective catalyst for isomerisation of methyl linoleate (cis-9,cis-12 (C18:2)) to CLA at 165 °C. Interestingly, no hydrogen pre-treatment of the catalyst or addition of hydrogen donors is required to achieve industrially relevant isomerisation productivities, namely, 0.7 g of CLA per litre of solvent per minute. Moreover, the biologically most active CLA isomers, namely, cis-9,trans-11, trans-10,cis-12 and trans-9,trans-11, were the main products, especially at low catalyst concentrations. Ex situ physicochemical characterisation with CO chemisorption, extended X-ray absorption fine structure measurements, transmission electron microscopy analysis, and temperature-programmed oxidation reveals the presence of highly dispersed RuO(2) species in Ru/Cs-USY(40).

  2. Phenol Tert-Butylation Catalyzed by Zeolite H-Mordenite

    Institute of Scientific and Technical Information of China (English)

    HAN Sen; LI Zhenhua; ZHANG Kui

    2005-01-01

    Para-tert-butyl phenol (p-TBP) and 2,4-di-tert-butyl phenol (2,4-DTBP) are widely used for the preparation of antioxidants. Zeolite catalysts showed good performance for the synthesis of p-TBP and 2,4-DTBP. In this work, zeolite H-mordenite (HM) catalyst was prepared and the alkylation of phenol with tert-butyl alcohol over zeolite HM catalyst was investigated at different reaction conditions. It is found that increasing temperature enhances the selectivity to p-TBP and the optimum reaction temperature for phenol conversion is 438 K. Increasing flow rate decreases phenol conversion apparently while the selectivity to p-TBP has a little increase. The suitable tert-butyl alcohol/phenol molar ratio is 2. Lower alcohol/phenol molar ratios are beneficial to p-TBP while higher ones are helpful for producing 2,4-DTBP.

  3. Vanadia supported on zeolites for SCR of NO by ammonia

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Riisager, Anders; Fehrmann, Rasmus

    2010-01-01

    Vanadia supported on zeolites were prepared and characterized by N-2 physisorption, FTIR. XRPD, and NH3-TPD methods. The influence of the Si/Al ratio on the total surface acidity of the catalysts as well as the optimum V2O5 content were studied and compared with the catalytic activity in the sele......Vanadia supported on zeolites were prepared and characterized by N-2 physisorption, FTIR. XRPD, and NH3-TPD methods. The influence of the Si/Al ratio on the total surface acidity of the catalysts as well as the optimum V2O5 content were studied and compared with the catalytic activity......, acidity and micropore structure of the support. Apparently the support hosted the potassium oxide on the acid sites, thereby protecting the active vanadium species from poisoning. Zeolite based catalysts might therefore prove useful for SCR of NO in alkali-containing flue gases from, e.g. biomass fired...

  4. Lithium modified zeolite synthesis for conversion of biodiesel-derived glycerol to polyglycerol

    Energy Technology Data Exchange (ETDEWEB)

    Ayoub, Muhammad, E-mail: muhammad.ayoub@petronas.com.my [Department of Chemical Engineering, Universiti Teknologi PETRONAS, 31750, Tronoh, Perak, Malaysia and School of Chemical Engineering, Universiti Sains Malaysia, 43000, Pinang (Malaysia); Abdullah, Ahmad Zuhairi, E-mail: chzuhairi@usm.my [School of Chemical Engineering, Universiti Sains Malaysia, 43000, Pinang (Malaysia); Inayat, Abrar, E-mail: abrar.inayat@petronas.com.my [Department of Chemical Engineering, Universiti Teknologi PETRONAS, 31750, Tronoh, Perak (Malaysia)

    2014-10-24

    Basic zeolite has received significant attention in the catalysis community. These zeolites modified with alkaline are the potential replacement for existing zeolite catalysts due to its unique features with added advantages. The present paper covers the preparation of lithium modified zeolite Y (Li-ZeY) and its activity for solvent free conversion of biodiesel-derived glycerol to polyglycerol via etherification process. The modified zeolite was well characterized by X-ray diffraction (XRD), Scanning Electron Microscope (SEM) and Nitrogen Adsorption. The SEM images showed that there was no change in morphology of modified zeolite structure after lithium modification. XRD patterns showed that the structure of zeolite was sustained after lithium modification. The surface properties of parent and modified zeolite was also observed N{sub 2} adsortion-desorption technique and found some changes in surface area and pore size. In addition, the basic strength of prepared materials was measured by Hammet indicators and found that basic strength of Li-ZeY was highly improved. This modified zeolite was found highly thermal stable and active heterogamous basic catalyst for conversion of solvent free glycerol to polyglycerol. This reaction was conducted at different temperatures and 260 °C was found most active temperature for this process for reaction time from 6 to 12 h over this basic catalyst in the absence of solvent.

  5. Performance of modified H-ZSM-5 zeolite for dehydration of methanol to dimethyl ether

    Energy Technology Data Exchange (ETDEWEB)

    Hassanpour, Samaneh; Taghizadeh, Majid [Department of chemical engineering, Babol University of Technology, P.O. Box 484, 4714871167 Babol (Iran); Yaripour, Fereydoon [Catalyst Research Group, Petrochemical Research and Technology Company, National Petrochemical Company, Tehran (Iran)

    2010-10-15

    The conversion of methanol to dimethyl ether was carried out over various commercial zeolites and modified H-ZSM-5 catalysts to evaluate their catalytic performance. A series of commercially available zeolite samples were used for vapor-phase dehydration of methanol to DME. Catalyst screening tests were performed in a fixed-bed reactor under the same operating conditions (T = 300 S, P = 16 barg, WHSV = 3.8 h{sup -1}). It was found that all the H-form zeolite catalysts in this study were active and selective for DME synthesis. According to the experimental results MDHC-1 catalyst exhibited the highest activity in dehydration of methanol. After finding the most active catalyst, the H-MFI90 zeolite was modified with Na content varying from 0 to 120 mol%, via wet-impregnation method to further improve its selectivity. All of catalysts were characterized by BET, XRD, NH{sub 3}-TPD, ICP, TGA, SEM, FT-IR and TPH techniques. It was found that these materials affected activity of MDHC-1 zeolite by changing its acidity. Ultimately, among all the catalysts studied, Na{sub 100}-modified H-MFI90 zeolite exhibited optimum activity, selectivity and stability at methanol dehydration reaction. (author)

  6. Characterization of the acid properties of tungsten/zirconia catalysts using adsorption microcalorimetry and n-pentane isomerization activity

    Energy Technology Data Exchange (ETDEWEB)

    Vartuli, J.C.; Santiesteban, J.G.; Traverso, P.; Cardona-Martinez, N.; Chang, C.D.; Stevenson, S.A.

    1999-10-01

    Ammonia adsorption microcalorimetry was conducted on various solid acid tungsten/zirconia catalysts prepared by different techniques. The calorimetric data were compared to catalytic test results using n-pentane isomerization as a measure of acid activity. The results show that (1) the co-precipitation method of making the tungsten/zirconia catalyst produces a greater number of acidic sites than impregnating tungsten on hydrous zirconia, resulting in a more active catalyst, and (2) the addition of small amounts of iron to the tungsten/zirconia catalyst increases the acid site strength as determined by ammonia adsorption and improves the paraffin isomerization activity. The calorimetry data indicate that the acid site strength of the tungsten/zirconia materials is similar to or slightly higher than that found in zeolites or sulfated zirconia and is comparable to sulfuric acid. However, the paraffin isomerization activity results suggest that the acid sites of the tungsten/zirconia catalyst should be about four orders of magnitude more active than that of zeolite {beta} on the basis of turnover frequency. Their experimental results indicate a lack of correlation between the heat of ammonia adsorption with catalytic activity. Comparisons of catalytic activity between materials based entirely on acid strength may not be valid, and kinetic probes would be more appropriate.

  7. Controlling chemistry with cations: photochemistry within zeolites.

    Science.gov (United States)

    Ramamurthy, V; Shailaja, J; Kaanumalle, Lakshmi S; Sunoj, R B; Chandrasekhar, J

    2003-08-21

    The alkali ions present in the supercages of zeolites X and Y interact with included guest molecules through quadrupolar (cation-pi), and dipolar (cation-carbonyl) interactions. The presence of such interactions can be inferred through solid-state NMR spectra of the guest molecules. Alkali ions, as illustrated in this article, can be exploited to control the photochemical and photophysical behaviors of the guest molecules. For example, molecules that rarely phosphoresce can be induced to do so within heavy cation-exchanged zeolites. The nature (electronic configuration) of the lowest triplet state of carbonyl compounds can be altered with the help of light alkali metal ions. This state switch (n pi*-pi pi*) helps to bring out reactivity that normally remains dormant. Selectivity obtained during the singlet oxygen oxidation of olefins within zeolites illustrates the remarkable control that can be exerted on photoreactions with the help of a confined medium that also has active sites. The reaction cavities of zeolites, like enzymes, are not only well-defined and confined, but also have active sites that closely guide the reactant molecule from start to finish. The examples provided here illustrate that zeolites are far more useful than simple shape-selective catalysts.

  8. Catalytic Performance of Fe/H-beta Catalyst Modified by Mn for NOx Decomposition at Low Temperature%Mn改性Fe/H-beta催化剂的低温催化分解NOx的研究

    Institute of Scientific and Technical Information of China (English)

    潘华; 宋华丰

    2012-01-01

    通过Mn改性制备了Fe和Mn的质量比为1且Fe和Mn的质量分数均为5% (5%Fe-5%Mn/H-beta)的催化剂,通过氢气程序升温还原(H2-TPR)比较分析了Fe-Mn/H-beta、Fe/H-beta和Mn/H-beta催化剂中Fe和Mn的化学形态,考察了O2、SO2和H2O等反应条件对Fe-Mn/H-beta催化剂低温催化分解NOx的影响.结果表明,相比Fe/H-beta和Mn/H-beta,Fe-Mn/H-beta 催化剂在富氧和低温条件下具有较好的催化活性,其中623 K下催化剂的活性最高,NOx的转化率达到45%左右.Fe-Mn/H-beta催化剂中Fe和Mn的共存提高了Fe2O3和MnO2的含量.氧的存在促进了NOx催化分解,水蒸气和SO2对NOx催化分解有一定的抑制作用.%Direct decomposition of NOX was investigated with 5% Fe-5% Mn/H-beta catalysts with equal weight of Mn and Fe. The chemical states of Fe and Mn in Fe-Mn/H-beta, Fe/H-be-ta, and Mn/H-beta catalysts were characterized by H2-TPR. The effects of O2, SO2 and H20 on decomposition of NOX at low temperature with 5 %Fe-5% Mn/H-beta catalysts were examined. The results indicate that the activity of Fe-Mn/H-beta is higher than that of Fe/H-beta or Mn/H-beta at rich oxygen and low temperature from 573 K to 673 K. The maximum NO* conversion is about 45% with 5 %Fe-5%Mn/H-beta at 623 K. The presence of Fe in Fe-Mn/H-beta enhances the transformation of Mn3+ ions into Mn4+ ions, and the addition of Mn increases the amount of Fe2O3 in Fe-Mn/H-beta. In addition, O2 inhibition is not observed in NOX decomposition with Fe-Mn/H-beta while the presence of H2O and SO2 inhibits the activity of Fe-Mn/H-beta.

  9. Isomerisation of c4-c6 aldoses with zeolites

    DEFF Research Database (Denmark)

    2014-01-01

    The present invention relates to isomerization of C4-C6 aldoses to their corresponding C4-C6 ketoses. In particular, the invention concerns isomerization of C4-C6 aldoses over solid zeolite catalysts free of any metals other than aluminum, in the presence of suitable solvent(s) at suitable elevated...... temperatures. C6 and C5 aldose sugars such as glucose and xylose, which are available in large amounts from biomass precursors, are isomerized to fructose and xylulose respectively, in a one or two-step process over inexpensive commercially available zeolite catalysts, containing aluminum as the only metal...

  10. Hierarchical zeolites from class F coal fly ash

    Science.gov (United States)

    Chitta, Pallavi

    Fly ash, a coal combustion byproduct is classified as types class C and class F. Class C fly ash is traditionally recycled for concrete applications and Class F fly ash often disposed in landfills. Class F poses an environmental hazard due to disposal and leaching of heavy metals into ground water and is important to be recycled in order to mitigate the environmental challenges. A major recycling option is to reuse the fly ash as a low-cost raw material for the production of crystalline zeolites, which serve as catalysts, detergents and adsorbents in the chemical industry. Most of the prior literature of fly ash conversion to zeolites does not focus on creating high zeolite surface area zeolites specifically with hierarchical pore structure, which are very important properties in developing a heterogeneous catalyst for catalysis applications. This research work aids in the development of an economical process for the synthesis of high surface area hierarchical zeolites from class F coal fly ash. In this work, synthesis of zeolites from fly ash using classic hydrothermal treatment approach and fusion pretreatment approach were examined. The fusion pretreatment method led to higher extent of dissolution of silica from quartz and mullite phases, which in turn led to higher surface area and pore size of the zeolite. A qualitative kinetic model developed here attributes the difference in silica content to Si/Al ratio of the beginning fraction of fly ash. At near ambient crystallization temperatures and longer crystallization times, the zeolite formed is a hierarchical faujasite with high surface area of at least 360 m2/g. This work enables the large scale recycling of class F coal fly ash to produce zeolites and mitigate environmental concerns. Design of experiments was used to predict surface area and pore sizes of zeolites - thus obviating the need for intense experimentation. The hierarchical zeolite catalyst supports tested for CO2 conversion, yielded hydrocarbons

  11. Efficient Production of Hydrogen from Decomposition of Formic Acid over Zeolite Incorporated Gold Nanoparticles

    DEFF Research Database (Denmark)

    Gallas-Hulin, Agata; Mielby, Jerrik Jørgen; Kegnæs, Søren

    2016-01-01

    Formic acid has a great potential as a safe and convenient source of hydrogen for sustainable chemical synthesis and renewable energy storage. Here, we report a heterogeneous gold nanoparticles catalyst for efficient production of hydrogen from vapor phase decomposition of formic acid using zeolite...... sintering stability. Based on these results, we believe that incorporation of metal nanoparticles in zeolites may find use as highly active and selective heterogeneous catalysts for the production of hydrogen in future renewable energy applications....

  12. Deuteriation exchange (with the deuteriated catalyst surface) and the ratio of dehydrogenation and dehydration of. cap alpha. - and. beta. -substituted ethanols on basic oxides

    Energy Technology Data Exchange (ETDEWEB)

    Thomke, K.

    1977-01-01

    The pulsed reactions of ethanol, 1- and 2-propanol, 1- and 2-butanol, 2-methyl-2-propanol, and 3-pentanol on deuteriated magnesium, samarium, thorium, and lanthanum oxides showed that no deuterium was incorporated at a carbon of 2-methyl-2-propanol (i.e., that the reaction did not proceed by the E1cB mechanism); that all the secondary alcohols formed olefins and ketones and incorporated deuterium only in the ..beta..-position; and that primary alcohols formed olefins and aldehydes on all catalysts except lanthanum oxide (which catalyzed only dehydration of primary alcohols) and incorporated deuterium in the ..cap alpha..-position on magnesium and thorium oxide. The mechanism is discussed. Table.

  13. Quantitative 3D Fluorescence Imaging of Single Catalytic Turnovers Reveals Spatiotemporal Gradients in Reactivity of Zeolite H-ZSM-5 Crystals upon Steaming

    NARCIS (Netherlands)

    Ristanovic, Zoran|info:eu-repo/dai/nl/328233005; Hofmann, Jan P.|info:eu-repo/dai/nl/355351110; De Cremer, Gert; Kubarev, Alexey V.; Rohnke, Marcus; Meirer, Florian; Hofkens, Johan; Roeffaers, Maarten B. J.; Weckhuysen, Bert M.|info:eu-repo/dai/nl/285484397

    2015-01-01

    Optimizing the number, distribution, and accessibility of Bronsted acid sites in zeolite-based catalysts is of a paramount importance to further improve their catalytic performance. However, it remains challenging to measure real-time changes in reactivity of single zeolite catalyst particles by ens

  14. Catalysis on Interface of Nano-oxide and Nano-zeolite

    Institute of Scientific and Technical Information of China (English)

    K.Ito; F.Jan; S.Asaoka

    2007-01-01

    1 Results The catalysts which can efficiently hydro-reform higher n-paraffin to lower isoparaffins for environmentally-friendly gasoline were studied. The catalysts were examined by the conversion of n-hexadecane, n-C16H34 to i-C6H14—i-C10H22.The tri-modally nano-porous catalysts composed of (Ni-Mo)/[γ-Al2O3], nano-oxide, and nano-crystalline zeolite had some active and selective performance because of the interface between nano-oxide and nano-zeolite. The catalyst composed of nano-crystalline MFI or BE...

  15. Photocatalytic Activity of TiO2 Coating on Natural Feather Zeolite in Degradation of Orthomonochlorphenol

    Institute of Scientific and Technical Information of China (English)

    CHEN Liang; ZHANG Zhi-xiang; CHEN Dong-hui

    2006-01-01

    TiO2 coatings on natural feather zeolite are respectively prepared by a collosol (Sol-gel) method and two powder coating methods with deionized water or dehydrated ethanol as a dispersant. During degradation of orthomonochlorphenol solutions by ultraviolet, the strong adsorption capability of the zeolite results in increased concentration of substrate on its surface. The TiO2 film coated on feather zeolite further enhances the photocatalytic activity. The TiO2 film on the zeolite prepared by the Sol-gel method is found more effective as a catalyst than that by two powder coating methods.

  16. A multisite molecular mechanism for Baeyer-Villiger oxidations on solid catalysts using environmentally friendly H2O2 as oxidant.

    Science.gov (United States)

    Boronat, Mercedes; Corma, Avelino; Renz, Michael; Sastre, Germán; Viruela, Pedro M

    2005-11-18

    The molecular mechanism of the Baeyer-Villiger oxidation of cyclohexanone with hydrogen peroxide catalyzed by the Sn-beta zeolite has been investigated by combining molecular mechanics, quantum-chemical calculations, spectroscopic, and kinetic techniques. A theoretical study of the location of Sn in zeolite beta was performed by using atomistic force-field techniques to simulate the local environment of the active site. An interatomic potential for Sn/Si zeolites, which allows the simulation of zeolites containing Sn in a tetrahedral environment, has been developed by fitting it to the experimental properties of quartz and SnO2(rutile). The tin active site has been modeled by means of a Sn(OSiH3)3OH cluster, which includes a defect in the framework that provides the flexibility necessary for the interaction between the adsorbates and the Lewis acid center. Two possible reaction pathways have been considered in the computational study, one of them involving the activation of the cyclohexanone carbonyl group by Sn (1) and the other one involving hydrogen peroxide being activated through the formation of a tin-hydroperoxo intermediate (2). Both the quantum-chemical results and the kinetic study indicate that the reaction follows mechanism 1, and that the catalyst active site consists of two centers: the Lewis acid Sn atom to which cyclohexanone has to coordinate, and the oxygen atom of the Sn-OH group that interacts with H2O2 forming a hydrogen bond.

  17. Exploring green catalysts for production of biofuels and value added chemicals for renewable and sustainable energy future

    Science.gov (United States)

    Budhi, Sridhar

    Porous silica have attracted significant attention in the past few decades due to their unique textural properties. They were extensively investigated for applications in catalysis, separation, environmental remediation and drug delivery. We have investigated the porous metal incorporated silica in the synthetic as well as catalytic perspectives. The synthesis of metal incorporated mesoporous silica via co-condensation such as SBA-15, KIT-5 are still challenging as it involves acidic synthetic route. Synthesis in high acidity conditions affects the incorporation of metal in silica due to high dissolution of metal precursors and breaking of metal oxygen and silica bond. The research presented here demonstrates an efficient way to incorporate metals by addition of diammonium hydrogen phosphate along with metal precursor during the synthesis. The incorporation efficiency has increased 2-3 times with this approach. Catalytic studies were performed to support our hypothesis. Such synthesized molybdenum incorporated mesoporous silica were investigated as catalyst for fast pyrolysis. When molydenum incorporated in silica was used as catalyst for fast pyrolysis of pine, it selectively produced furans (furan, methylfuran and dimethylfuran). Furans are considered value-added chemicals and can be used as a blendstock for diesel/jet grade fuel. The catalyst was very stable to harsh pyrolysis conditions and had a longer life before deactivation when compared with traditional zeolites. Further, this catalyst did not produce aromatic hydrocarbons in significant yields unlike zeolites. The origin of the furans was determined to be biopolymer cellulose and the selectivity for furans are attributed to low catalyst acidity. The effect of silica to alumina ratio (SAR) of beta-zeolite was investigated ranging to elucidate the relationship between the of number of acid sites on product speciation and catalyst deactivation on catalysts supplied by Johnson Matthey. The catalyst with low

  18. The Influence of Zeolites on Radical Formation During Lignin Pyrolysis.

    Science.gov (United States)

    Bährle, Christian; Custodis, Victoria; Jeschke, Gunnar; van Bokhoven, Jeroen A; Vogel, Frédéric

    2016-09-01

    Lignin from lignocellulosic biomass is a promising source of energy, fuels, and chemicals. The conversion of the polymeric lignin to fuels and chemicals can be achieved by catalytic and noncatalytic pyrolysis. The influence of nonporous silica and zeolite catalysts, such as silicalite, HZSM5, and HUSY, on the radical and volatile product formation during lignin pyrolysis was studied by in situ high-temperature electron paramagnetic resonance spectroscopy (HTEPR) as well as GC-MS. Higher radical concentrations were observed in the samples containing zeolite compared to the sample containing only lignin, which suggests that there is a stabilizing effect by the inorganic surfaces on the formed radical fragments. This effect was observed for nonporous silica as well as for HUSY, HZSM5, and silicalite zeolite catalysts. However, the effect is far larger for the zeolites owing to their higher specific surface area. The zeolites also showed an effect on the volatile product yield and the product distribution within the volatile phase. Although silicalite showed no effect on the product selectivity, the acidic zeolites such as HZSM5 or HUSY increased the formation of deoxygenated products such as benzene, toluene, xylene (BTX), and naphthalene.

  19. An Overview of Recent Development in Composite Catalysts from Porous Materials for Various Reactions and Processes

    Directory of Open Access Journals (Sweden)

    Zaiku Xie

    2010-05-01

    Full Text Available Catalysts are important to the chemical industry and environmental remediation due to their effective conversion of one chemical into another. Among them, composite catalysts have attracted continuous attention during the past decades. Nowadays, composite catalysts are being used more and more to meet the practical catalytic performance requirements in the chemical industry of high activity, high selectivity and good stability. In this paper, we reviewed our recent work on development of composite catalysts, mainly focusing on the composite catalysts obtained from porous materials such as zeolites, mesoporous materials, carbon nanotubes (CNT, etc. Six types of porous composite catalysts are discussed, including amorphous oxide modified zeolite composite catalysts, zeolite composites prepared by co-crystallization or overgrowth, hierarchical porous catalysts, host-guest porous composites, inorganic and organic mesoporous composite catalysts, and polymer/CNT composite catalysts.

  20. Advance in heterogeneous catalysts for styrene epoxidation to styrene oxide with molecular oxygen%分子氧氧化苯乙烯制备环氧苯乙烷的多相催化剂研究进展

    Institute of Scientific and Technical Information of China (English)

    杨瑞云; 王宪沛; 李文; 李小安; 闫俊; 张辉辉; 刘卫涛

    2013-01-01

    综述了分子氧氧化苯乙烯制备环氧苯乙烷的多相催化剂研究进展,重点介绍了Co系催化剂在苯乙烯环氧化方面的应用.其中,负载在Beta型分子筛上的Co-Beta催化剂具有较高的催化活性、选择性及稳定性.%The latest research progress in the heterogeneous catalysts for epoxidation of styrene to styrene oxide by molecular oxygen was reviewed,especially cobalt catalyst,among which Co-beta catalysts supported on beta zeolites exhibited higher catalytic activity,selectivity and stability.

  1. Metallocene supported core@LDH catalysts for slurry phase ethylene polymerisation.

    Science.gov (United States)

    Buffet, Jean-Charles; Byles, Coral F H; Felton, Ryan; Chen, Chunping; O'Hare, Dermot

    2016-03-14

    We report the synthesis of solid catalysts based on a zirconocene supported on either silica@AMO-LDH or zeolite@AMO-LDH for the slurry phase polymerisation of ethylene. The hybrid catalysts demonstrate synergistic effects in which the polymerisation activity is up to three times higher than the zirconocene supported on analogous single phase silica or zeolite supports.

  2. Effect of hierarchical porosity and phosphorus modification on the catalytic properties of zeolite Y

    Science.gov (United States)

    Li, Wenlin; Zheng, Jinyu; Luo, Yibin; Da, Zhijian

    2016-09-01

    The zeolite Y is considered as a leading catalyst for FCC industry. The acidity and porosity modification play important roles in determining the final catalytic properties of zeolite Y. The alkaline treatment of zeolite Y by dealumination and alkaline treatment with NaOH and NaOH&TBPH was investigated. The zeolites were characterized by X-ray diffraction, low-temperature adsorption of nitrogen, transmission electron microscope, NMR, NH3-TPD and IR study of acidity. Accordingly, the hierarchical porosity and acidity property were discussed systematically. Finally, the catalytic performance of the zeolites Y was evaluated in the cracking of 1,3,5-TIPB. It was found that desilication with NaOH&TBPH ensured the more uniform intracrystalline mesoporosity with higher microporosity, while preserving higher B/L ratio and moderate Brønsted acidities resulting in catalysts with the most appropriated acidity and then with better catalytic performance.

  3. Modification of acidity of Mo-Fe/HZSM-5 zeolite via argon plasma treatment

    Institute of Scientific and Technical Information of China (English)

    Xinli ZHU; Kailu YU; Dangguo CHENG; Yueping ZHANG; Qing XIA; Changjun LIU

    2008-01-01

    The NH3-TPD characterization was conducted to confirm that the acidity of Mo-Fe/HZSM-5 zeolite could be selectively modified via the glow discharge plasma treatment. The plasma catalyst treatment could totally change the distribution of aromatic products with higher methane conversion compared to the untreated catalyst. Some polycyclic aromatics such as anthracene, pyrene and phenanthrene were also produced over the plasma treated catalyst, in addition to benzene, toluene and naphthalene, which were normally obtained over the untreated catalyst.

  4. Zeolite and zeotype-catalysed transformations of biofuranic compounds

    DEFF Research Database (Denmark)

    Li, Hu; Yang, Song; Riisager, Anders

    2016-01-01

    ,5-furandicarboxylic acid can be obtained from hexoses and pentoses via selective dehydration and subsequent etherification, hydrogenation, oxidation reactions, which show great potential for industrial applications to replace petroleum-based chemicals and fuels. Zeolite and zeotype micro- and mesoporous materials...... with tuneable acidity, good thermal stability and shape-selectivity have recently emerged as promising solid catalysts, exhibiting superior catalytic performance to other heterogeneous catalysts. This review focuses on the synthesis of biomass-derived furanic compounds catalysed by zeolitic materials, firstly...... introducing zeolite-catalysed hydrolysis of di-, oligo- and polysaccharides and isomerization reactions of monomeric sugars. Subsequently, the catalytic dehydration reactions of hexoses and pentoses to obtain HMF and furfural are reported. Particularly, a variety of reaction pathways towards upgrading...

  5. Activities of aluminum forms of zeolites and zeolite-containing aluminosilicates in phenol arylalkylation by styrene

    Energy Technology Data Exchange (ETDEWEB)

    Kurashev, M.V.; Kolesnichenko, N.V.; Romanovskii, B.V.; Lokshin, B.V.

    1979-03-01

    The activities of aluminum forms of zeolites and zeolite-containing aluminosilicates in phenol arylalkylation by styrene were studied in a flow microreactor at 250/sup 0/C, 1 atm, 4:1 phenol-styrene, and 2.6 sec contact time. The aluminum-exchanged forms of a NaY zeolite and a zeolite-containing amorphous aluminosilicate (the Soviet commercial AShNTs-3 grade) were prepared by the K. M. Wang technique and some of the samples were pretreated by phenol at 250/sup 0/C and 2 atm for two hours. The AShNTs-3 and Al/AShNTs-3 catalysts showed maximum steady-state activities in terms of over-all styrene conversion (67.6 and 46.7Vertical Bar3<, respectively) and the combined yield of 2- and 4-(..cap alpha..-methylbenzyl)phenols (64.1 and 32.2Vertical Bar3<, respectively). The AlNaY zeolite rapidly and irreversibly deactivated, and pure amorphous aluminosilicate (AAS) showed relatively low activity. The pretreatment with phenol improved the activities of the aluiminum forms and increased the ortho-to-para isomer ratio of the alkylate from 2.74 to 4.33 for Al/AShNTs-3 and from 2.37 to 4.00 for AAS, probably because of the formation of active surface aluminum phenolate structures, but deteriorated the catalytic properties of AShNTs-3.

  6. Hierarchical Porous ZSM-5 Zeolite Synthesized by in situ Zeolitization and Its Coke Deposition Resistance in Aromatization Reaction

    Institute of Scientific and Technical Information of China (English)

    张珂; 柳云骐; 赵晋翀; 刘晨光

    2012-01-01

    Hierarchical ZSM-5 zeolites with micro-, meso- and macroporosity were prepared from diatomite zeolitization through a vapor-phase transport process on solid surfaces. The aromatization performance of the catalysts was in- vestigated on a fixed bed reactor by using FCC gasoline as feedstock. The crystal phase, morphology, pore struc- tures, acidity and coke depositions of the hierarchical ZSM-5 zeolites were characterized by means of X-ray diffrac- tion (XRD), scanning electron microscope (SEM), N2 adsorption/desorption, Fourier transform infrared (FT-IR) and thermogravimetry-mass spectrogram (TG-MS), respectively. The results show that the prepared hierarchical ZSM-5 zeolite possesses excellent porosity and high crystallinity, displaying an improved aromatization performance and carbon deposition resistance due to its meso- and macroporous structures.

  7. Conversion of Isoprenoid Oil by Catalytic Cracking and Hydrocracking over Nanoporous Hybrid Catalysts

    Directory of Open Access Journals (Sweden)

    Toshiyuki Kimura

    2012-01-01

    Full Text Available In order to produce petroleum alternatives from biomass, a significant amount of research has been focused on oils from microalgae due to their origin, which would not affect food availability. Nanoporous hybrid catalysts composed of ns Al2O3 and zeolites have been proven to be very useful compared to traditional catalysts in hydrotreating (HT, hydrocracking (HC, and catalytic cracking (CC of large molecules. To evaluate the reaction scheme and products from model isoprenoid compounds of microalgae oil, nanoporous hybrid catalyst technologies (CC: ns Al2O3/H-USY and ns Al2O3/H-GaAlMFI; HC: [Ni-Mo/γ-Al2O3]/ns Al2O3/H-beta were studied. The major product from CC on ns Al2O3/H-USY was highly aromatic gasoline, while the product from HC was half-isoparaffinic/olefinic kerosene. Although more than 50 wt% of the products from HT/CC on the USY catalyst was liquefied petroleum gas due to overcracking, the product from HT/CC on the MFI catalyst was high-octane-number gasoline. Delightfully, the product from HT/HC was kerosene and its average number was 11, with more than 80 wt% being isoparaffinic. As a result, it was demonstrated that hydrotreating may convert isoprenoid oil from microalgae over nanoporous hybrid catalysts into a variety of products.

  8. Conversion of isoprenoid oil by catalytic cracking and hydrocracking over nanoporous hybrid catalysts.

    Science.gov (United States)

    Kimura, Toshiyuki; Liu, Chen; Li, Xiaohong; Maekawa, Takaaki; Asaoka, Sachio

    2012-01-01

    In order to produce petroleum alternatives from biomass, a significant amount of research has been focused on oils from microalgae due to their origin, which would not affect food availability. Nanoporous hybrid catalysts composed of ns Al₂O₃ and zeolites have been proven to be very useful compared to traditional catalysts in hydrotreating (HT), hydrocracking (HC), and catalytic cracking (CC) of large molecules. To evaluate the reaction scheme and products from model isoprenoid compounds of microalgae oil, nanoporous hybrid catalyst technologies (CC: ns Al₂O₃/H-USY and ns Al₂O₃/H-GaAlMFI; HC: [Ni-Mo/γ-Al₂O₃]/ns Al₂O₃/H-beta) were studied. The major product from CC on ns Al₂O₃/H-USY was highly aromatic gasoline, while the product from HC was half-isoparaffinic/olefinic kerosene. Although more than 50 wt% of the products from HT/CC on the USY catalyst was liquefied petroleum gas due to overcracking, the product from HT/CC on the MFI catalyst was high-octane-number gasoline. Delightfully, the product from HT/HC was kerosene and its average number was 11, with more than 80 wt% being isoparaffinic. As a result, it was demonstrated that hydrotreating may convert isoprenoid oil from microalgae over nanoporous hybrid catalysts into a variety of products.

  9. Mesoporous molecular sieve catalysts

    DEFF Research Database (Denmark)

    Højholt, Karen Thrane

    be used as solid acid catalysts but can also be used as a size-selective matrix. It was shown that it is possible to encapsulate 1-2 nm sized gold nanoparticles by silicalite-1 or ZSM-5 zeolite crystals thereby forming a sintering-stable and substrate size-selective oxidation catalyst. After carrying out...... calcination experiments, both in situ and ex situ indicated that the gold nanoparticles embedded in the crystals were highly stable towards sintering. The catalytic tests proved that the embedded gold nanoparticles were active in selective aldehyde oxidation and were only accessible through the micropores...

  10. Acetalization of furfural with zeolites under benign reaction conditions

    DEFF Research Database (Denmark)

    Rubio-Caballeroa, Juan Miguel; Shunmugavel, Saravanamurugan; Maireles-Torres, Pedro

    2014-01-01

    Acetalization is a viable method to protect carbonyl functionalities in organic compounds and offers apotential synthetic strategy for synthesizing derived chemicals. In this work, several families of commer-cial zeolites have been employed as solid acid catalysts in the acetalization of furfural...

  11. Computer Simulation of Zeolites : Adsorption, Diffusion and Dealumination

    NARCIS (Netherlands)

    Ban, S.

    2009-01-01

    Zeolites are microporous materials with pores that have about the same size as small molecules like water or benzene. They are important catalysts in the petrochemical industry, for example for catalytic cracking, and isomerization- and alkylation reactions. This thesis deals with molecular aspects

  12. Bifunctional Nanostructured Base Catalysts: Opportunities for BioFuels

    Energy Technology Data Exchange (ETDEWEB)

    Connor, William

    2010-12-30

    ABSTRACT This research studied and develop novel basic catalysts for production of renewable chemicals and fuels from biomass. We will focus on the development of unique porous structural-base catalysts formed by two techniques: from (mixed) metal-oxide bases and by nitrogen substitution for oxygen in zeolites. These catalysts will be compared to conventional solid base materials for aldol condensation, catalytic fast pyrolysis, and transesterification reactions. These reactions are important in processes that are currently being commercialized for production of fuels from biomass and will be pivotal in future biomass conversion to fuels and chemicals. Specifically, we have studied the aldol-condensation of acetone with furfural over oxides and zeolites, the conversion of sugars by rapid pyrolysis over zeolites and the trans-esterification of vegetable oil with methanol over mixed oxide catalysts. Our previous research has indicated that the base strength of framework nitrogen in nitrogen-substituted zeolites (NH-zeolites) is nearly twice as strong as in standard zeolites. Nitrogen substituted catalysts have been synthesized from several zeolites (including FAU, MFI, BEA, and LTL) using NH3 treatment.

  13. Catalytic pyrolysis of wheat bran for hydrocarbons production in the presence of zeolites and noble-metals by using TGA-FTIR method.

    Science.gov (United States)

    Lazdovica, K; Liepina, L; Kampars, V

    2016-05-01

    Pyrolysis of wheat bran with or without catalysts was investigated using TGA-FTIR method in order to determine the influence of zeolite and noble metal catalysts on the evolution profile and relative yield of the volatile compounds. The addition of all catalysts decreased the volatile matter of wheat bran from 76.3% to 75.9%, 73.9%, 73.5%, 69.7% and increased the solid residue from 18.0% to 18.4%, 20.4%, 20.8%, 24.6% under the catalyst of ZSM-5, 5% Pd/C, MCM-41, and 5% Pt/C. Noble-metal catalysts had higher activity for deoxygenation of compounds containing carbonyl, carboxyl, and hydroxyl groups than zeolites. Degradation of nitrogen containing compounds atom proceeded better in presence of zeolites. Noble-metal catalysts promoted formation of aromatics and changed the profiles of evolved compounds whereas zeolites advanced formation of aliphatics and olefins.

  14. Dual template synthesis of a highly mesoporous SSZ-13 zeolite with improved stability in the methanol-to-olefins reaction

    OpenAIRE

    Wu, Leilei; Degirmenci, Volkan; Magusin, Pieter; Szyja, Bartlomiej M; Hensen, Emiel J.M.

    2012-01-01

    The dual template synthesis of zeolite SSZ-13 by use of trimethyl-adamantanammonium hydroxide and a diquaternary-ammonium mesoporogen induces considerable mesoporosity without impeding zeolite microporosity. The strongly improved accessibility of Brønsted sites in mesoporous SSZ-13 increases its stability during application as an acid catalyst in the methanol-to-olefins reaction.

  15. Dual template synthesis of a highly mesoporous SSZ-13 zeolite with improved stability in the methanol-to-olefins reaction.

    Science.gov (United States)

    Wu, Leilei; Degirmenci, Volkan; Magusin, Pieter C M M; Szyja, Bartłomiej M; Hensen, Emiel J M

    2012-10-04

    The dual template synthesis of zeolite SSZ-13 by use of trimethyl-adamantanammonium hydroxide and a diquaternary-ammonium mesoporogen induces considerable mesoporosity without impeding zeolite microporosity. The strongly improved accessibility of Brønsted sites in mesoporous SSZ-13 increases its stability during application as an acid catalyst in the methanol-to-olefins reaction.

  16. Gold and gold-iron modified zeolites--towards the adsorptive deodourisation.

    Science.gov (United States)

    Sobczak, Izabela; Pawlowski, Hubert; Chmielewski, Jaroslaw; Ziolek, Maria

    2010-07-15

    Zeolites exhibiting different structures (Y, Beta, and ZSM-5) were modified with gold and iron and applied for odour adsorption from the air containing dibutyl sulphide (Bu(2)S) used as a representative odour producing compound. The structure of the zeolites used determines the rate of adsorption (higher on Y type zeolites and smaller on two other zeolites), whereas hydrophilicity affects the selectivity towards Bu(2)S adsorption increasing in the order: Yzeolite structure, Bu(2)S adsorption selectivity depends on the total acidity of zeolites which increases after iron modification. The texture and surface properties of the modified zeolites were studied by XRD, XPS, UV-vis, TEM, pyridine adsorption and FTIR, test reactions (acetonylacetone cyclisation, isopropanol decomposition).

  17. Utilization of biomass: Conversion of model compounds to hydrocarbons over zeolite H-ZSM-5

    DEFF Research Database (Denmark)

    Mentzel, Uffe Vie; Holm, Martin Spangsberg

    2011-01-01

    Zeolite catalyzed deoxygenation of small oxygenates present in bio-oil or selected as model compounds was performed under Methanol-to-Hydrocarbons (MTH) like reaction conditions using H-ZSM-5 as the catalyst. Co-feeding of the oxygenates with methanol generally decreases catalyst lifetime due to ...

  18. Synthesis of Modified β-Zeolite Under Microwave Irradiation and Its Use on Etherification

    Institute of Scientific and Technical Information of China (English)

    Ma Jun; Wang Haiyan; Hu Tingfang; Tian Yanwen; Zhou Tong; Qin Zhiwei

    2004-01-01

    β -zeolite was synthesized by using tetraethyl ammonium hydroxide as the template reagent and microwave radiation as the heat source. The effect of the sol composition and the radiation temperature on zeolite crystallinity was investigated. The zeolite was tested and compared with the commercial product, which was produced by conventional hydrothermal synthesis method. ,The physico-chemical properties of the synthesized samples, the specific surface area of the samples synthesized under microwave irradiation and pore volume measured by X-ray diffraction apparatus, were better than the conventional samples. The etherification experiment on FCC light naphtha in the presence of transition metals modified H β -zeolite, which was synthesized firstly under microwave irradiation, was studied in a fixed-bed reactor. The effect of catalyst preparation conditions on its activity, stability and the effect of reaction temperature, methanol/tertiary-carbon olefin molar ratio and liquid hourly space velocity on the etherification reaction were discussed. The experimental results showed that the different metals modified H β -zeolite had different etherification performances. And the conversion of tertiary carbon-olefins of the molybdenum modified H β zeolite, which was loaded at a concentration of 3 percents, was higher than that on 6.0 percent of H β zeolite. The modified H β zeolite catalysts possessed favorable prospects for its higher stability.

  19. Tailor and Control of Acidic Strength in Ordered Mesoporous Aluminosilicates by Using Preformed Zeolite Precursors

    Institute of Scientific and Technical Information of China (English)

    LIN,Sen(林森); WANG,Li-Feng(王利丰); HAN,Yu(韩宇); YU,Yi(于沂); DI,Yan(邸岩); WANG,Run-Wei(王润伟); JIANG,Da-Zhen(蒋大振); XIAO,Feng-Shou(肖丰收)

    2004-01-01

    The acidic strength of ordered mesoporous aluminosilicates of MAS-2, MAS-3, MAS-7 and MAS-9 and microporous crystals of Y, L, beta, and ZSM-5 zeolites was systemically investigated by temperature-programmed desorption of ammonia (NH3-TPD). Due to the use of preformed zeolite precursors of Y, L, beta and ZSM-5, the ordered mesoporous aluminosilicates with distinguished acidic strength were obtained, being dependent on the type of preformed zeolite precursors. Therefore, the acidic strength of these mesoporous aluminosilicates could be tailored and controlled.

  20. Zeolite Membrane Reactor for Water Gas Shift Reaction for Hydrogen Production

    Energy Technology Data Exchange (ETDEWEB)

    Lin, Jerry Y.S. [Arizona State Univ., Mesa, AZ (United States)

    2013-01-29

    Gasification of biomass or heavy feedstock to produce hydrogen fuel gas using current technology is costly and energy-intensive. The technology includes water gas shift reaction in two or more reactor stages with inter-cooling to maximize conversion for a given catalyst volume. This project is focused on developing a membrane reactor for efficient conversion of water gas shift reaction to produce a hydrogen stream as a fuel and a carbon dioxide stream suitable for sequestration. The project was focused on synthesizing stable, hydrogen perm-selective MFI zeolite membranes for high temperature hydrogen separation; fabricating tubular MFI zeolite membrane reactor and stable water gas shift catalyst for membrane reactor applications, and identifying experimental conditions for water gas shift reaction in the zeolite membrane reactor that will produce a high purity hydrogen stream. The project has improved understanding of zeolite membrane synthesis, high temperature gas diffusion and separation mechanisms for zeolite membranes, synthesis and properties of sulfur resistant catalysts, fabrication and structure optimization of membrane supports, and fundamentals of coupling reaction with separation in zeolite membrane reactor for water gas shift reaction. Through the fundamental study, the research teams have developed MFI zeolite membranes with good perm-selectivity for hydrogen over carbon dioxide, carbon monoxide and water vapor, and high stability for operation in syngas mixture containing 500 part per million hydrogen sulfide at high temperatures around 500°C. The research teams also developed a sulfur resistant catalyst for water gas shift reaction. Modeling and experimental studies on the zeolite membrane reactor for water gas shift reaction have demonstrated the effective use of the zeolite membrane reactor for production of high purity hydrogen stream.

  1. 分子筛催化剂晶化母液有效成分絮凝回收的研究%Study on the Method for the Recovery of Effective Components from Crystallized Mother Liquor of Zeolite Catalyst by Flocculation Method

    Institute of Scientific and Technical Information of China (English)

    栾国颜; 王建刚; 刘发; 曹立东

    2015-01-01

    确定了可见分光光度计法测定分子筛催化剂晶化母液和丙烯酸絮凝后清液的磷含量,实验比较研究了不同絮凝剂回收分子筛催化剂晶化母液中有效成分的效果,通过单因素实验重点研究了丙烯酸作为絮凝剂在不同的浓度、絮凝温度、絮凝时间等因素对絮凝效果的影响,实验确定的最佳絮凝条件为:10.0 mL母液,丙烯酸(98.75%)2.0 mL,温度22.2℃,反应时间6 s,磷回收率可达到为94.3%。%The phosphorus contents of the crystallized mother liquor of zeolite catalysts for the flocculants were determined quantitatively by spectrophotometer.The flocculation effects were compared for effective components from the crystallized mother liquor of zeolite catalysts.Based on flocculation experiments of acrylic acid, the flocculant concentration, flocculation temperature, flocculation time were investigated by single factor experiments.The results showed that the optimal flocculating conditions were 2.0 mL acrylic acid for 98.75%concentration added in 10 mL of the crystallized mother liquor, the flocculation temperature was controlled at 22.2℃, flocculation time was 6 s.The recovery efficiency for phosphorus contents of the mother liquor was 94.3%.

  2. A continuous flow strategy for the coupled transfer hydrogenation and etherification of 5-(hydroxymethyl)furfural using Lewis acid zeolites.

    Science.gov (United States)

    Lewis, Jennifer D; Van de Vyver, Stijn; Crisci, Anthony J; Gunther, William R; Michaelis, Vladimir K; Griffin, Robert G; Román-Leshkov, Yuriy

    2014-08-01

    Hf-, Zr- and Sn-Beta zeolites effectively catalyze the coupled transfer hydrogenation and etherification of 5-(hydroxymethyl)furfural with primary and secondary alcohols into 2,5-bis(alkoxymethyl)furans, thus making it possible to generate renewable fuel additives without the use of external hydrogen sources or precious metals. Continuous flow experiments reveal nonuniform changes in the relative deactivation rates of the transfer hydrogenation and etherification reactions, which impact the observed product distribution over time. We found that the catalysts undergo a drastic deactivation for the etherification step while maintaining catalytic activity for the transfer hydrogenation step. (119) Sn and (29) Si magic angle spinning (MAS) NMR studies show that this deactivation can be attributed to changes in the local environment of the metal sites. Additional insights were gained by studying effects of various alcohols and water concentration on the catalytic reactivity.

  3. Visualizing Dealumination of a Single Zeolite Domain in a Real-Life Catalytic Cracking Particle.

    Science.gov (United States)

    Kalirai, Sam; Paalanen, Pasi P; Wang, Jian; Meirer, Florian; Weckhuysen, Bert M

    2016-09-05

    Fluid catalytic cracking (FCC) catalysts play a central role in the chemical conversion of crude oil fractions. Using scanning transmission X-ray microscopy (STXM) we investigate the chemistry of one fresh and two industrially deactivated (ECAT) FCC catalysts at the single zeolite domain level. Spectro-microscopic data at the Fe L3 , La M5 , and Al K X-ray absorption edges reveal differing levels of deposited Fe on the ECAT catalysts corresponding with an overall loss in tetrahedral Al within the zeolite domains. Using La as a localization marker, we have developed a novel methodology to map the changing Al distribution of single zeolite domains within real-life FCC catalysts. It was found that significant changes in the zeolite domain size distributions as well as the loss of Al from the zeolite framework occur. Furthermore, inter- and intraparticle heterogeneities in the dealumination process were observed, revealing the complex interplay between metal-mediated pore accessibility loss and zeolite dealumination.

  4. Recent advances of pore system construction in zeolite-catalyzed chemical industry processes.

    Science.gov (United States)

    Shi, Jing; Wang, Yangdong; Yang, Weimin; Tang, Yi; Xie, Zaiku

    2015-12-21

    The kaleidoscopic applications of zeolite catalysts (zeo-catalysts) in petrochemical processes has been considered as one of the major accomplishments in recent decades. About twenty types of zeolite have been industrially applied so far, and their versatile porous architectures have contributed their most essential features to affect the catalytic efficiency. This review depicts the evolution of pore models in zeolite catalysts accompanied by the increase in industrial and environmental demands. The indispensable roles of modulating pore models are outlined for zeo-catalysts for the enhancement of their catalytic performances in various industrial processes. The zeolites and related industrial processes discussed range from the uni-modal micropore system of zeolite Y (12-ring micropore, 12-R) in fluid catalytic cracking (FCC), zeolite ZSM-5 (10-R) in xylene isomerization and SAPO-34 (8-R) in olefin production to the multi-modal micropore system of MCM-22 (10-R and 12-R pocket) in aromatic alkylation and the hierarchical pores in FCC and catalytic cracking of C4 olefins. The rational construction of pore models, especially hierarchical features, is highlighted with a careful classification from an industrial perspective accompanied by a detailed analysis of the theoretical mechanisms.

  5. Diagram of Zeolite Crystals

    Science.gov (United States)

    2003-01-01

    The Center for Advanced Microgravity Materials Processing (CAMMP) in Cambridge, MA, a NASA-sponsored Commercial Space Center, is working to improve zeolite materials for storing hydrogen fuel. CAMMP is also applying zeolites to detergents, optical cables, gas and vapor detection for environmental monitoring and control, and chemical production techniques that significantly reduce by-products that are hazardous to the environment. Depicted here is one of the many here complex geometric shapes which make them highly absorbent. Zeolite experiments have also been conducted aboard the International Space Station

  6. The growth of carbon nanotubes on montmorillonite and zeolite (clinoptilolite)

    Energy Technology Data Exchange (ETDEWEB)

    Kadlecikova, M. [Department of Microelectronics, Faculty of Electrical Engineering and Information Technology, Slovak University of Technology, Ilkovicova 3, 812 19 Bratislava (Slovakia); Breza, J. [Department of Microelectronics, Faculty of Electrical Engineering and Information Technology, Slovak University of Technology, Ilkovicova 3, 812 19 Bratislava (Slovakia)], E-mail: juraj.breza@stuba.sk; Jesenak, K.; Pastorkova, K.; Luptakova, V. [Department of Inorganic Chemistry, Faculty of Natural Sciences, Comenius University, Mlynska Dolina, 842 15 Bratislava (Slovakia); Kolmacka, M.; Vojackova, A. [Department of Microelectronics, Faculty of Electrical Engineering and Information Technology, Slovak University of Technology, Ilkovicova 3, 812 19 Bratislava (Slovakia); Michalka, M. [International Laser Centre, Ilkovicova 3, 812 19 Bratislava (Slovakia); Vavra, I. [Institute of Electrical Engineering, Slovak Academy of Sciences, Dubravska Cesta 9, 841 04 Bratislava (Slovakia); Krizanova, Z. [Department of Microelectronics, Faculty of Electrical Engineering and Information Technology, Slovak University of Technology, Ilkovicova 3, 812 19 Bratislava (Slovakia)

    2008-06-15

    Synthesis of carbon nanotubes described in the present work is based on activation of methane in a hot filament CVD reactor and subsequent creation of nanostructures on a catalyst pre-treated polished surface of silicon. An essential step of the synthesis is the use of natural minerals as catalysts. We have studied the catalyst parameters, the way of its application and the amount of Fe{sup 3+} cations on the surface of aluminosilicates on the quality of the grown nanotube layers. The growth of carbon nanotubes catalyzed by montmorillonite and zeolite (clinoptilolite) was confirmed by scanning electron microscopy and Raman spectroscopy.

  7. The growth of carbon nanotubes on montmorillonite and zeolite (clinoptilolite)

    Science.gov (United States)

    Kadlečíková, M.; Breza, J.; Jesenák, K.; Pastorková, K.; Luptáková, V.; Kolmačka, M.; Vojačková, A.; Michalka, M.; Vávra, I.; Križanová, Z.

    2008-06-01

    Synthesis of carbon nanotubes described in the present work is based on activation of methane in a hot filament CVD reactor and subsequent creation of nanostructures on a catalyst pre-treated polished surface of silicon. An essential step of the synthesis is the use of natural minerals as catalysts. We have studied the catalyst parameters, the way of its application and the amount of Fe 3+ cations on the surface of aluminosilicates on the quality of the grown nanotube layers. The growth of carbon nanotubes catalyzed by montmorillonite and zeolite (clinoptilolite) was confirmed by scanning electron microscopy and Raman spectroscopy.

  8. Catalytic conversion of ethanol on H-Y zeolite

    Directory of Open Access Journals (Sweden)

    Čegar Nedeljko

    2005-01-01

    Full Text Available The catalytic activity of the H-form of synthetic zeolite NaY was examined in this study. The catalytic activity was determined according to the rate of ethanol conversion in a gas phase in the static system. In the conversion of ethanol on synthetic NaY zeolite at 585, 595, and 610 K, on which the reaction develops at an optimal rate, ethene and diethyl ether are evolved in approximately the same quantity. After transforming the NaY zeolite into the H-form, its catalytic activity was extremely increases so, the reaction develops at a significantly lower temperature with a very large increase in the reaction rate. The distribution of the products also changes, so that at lower temperatures diethyl ether is elvolved in most cases, and the development of ethene is favored at higher ones, and after a certain period of time there is almost complete conversion of ethanol into ethene. The increase in catalytic activity, as well as the change of selectivity of conversion of ethanol on the H-form of zeolite, is the result of removing Na+ cations in the NaY zeolite, so that more acidic catalyst is obtained which contains a number of acidic catalytically active centers, as well as a more powerful one compared to the original NaY zeolite.

  9. Fries Rearrangement of Phenyl Acetate over Solid Acid Catalyst

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    A silica-supported zirconium based solid acid (ZS) has been used as catalyst for the Fries rearrangement of phenyl acetate (PA). The catalyst showed a higher PA conversion activity and a much higher selectivity for o-hydroxyacetophenone (o-HAP) than for strongly acidic zeolite catalysts. The supported catalyst was characterized by XRD, IR, XPS, pyridine-TPD and the surface area measurements. The catalytic properties were influenced significantly by pretreatment temperature.

  10. Fries Rearrangement of Phenyl Acetate over Solid Acid Catalyst

    Institute of Scientific and Technical Information of China (English)

    CanXiongGUO; YanLIU; 等

    2002-01-01

    A silica-supported zirconium based solid acid (ZS) has been used as catalyst for the Fries rearrangement of phenyl acetate (PA). The catalyst showed a higher PA conversion activity and a much higher selectivity for o-hydroxyacetophenone (o-HAP) than for strongly acidic zeolite catalysts. The supported catalyst was characterized by XRD,IR,XPS,pyridine-TPD and the surface area measurements. The catalytic properties were influenced significantly by pretreatment temperature.

  11. Composite zeolite membranes

    Science.gov (United States)

    Nenoff, Tina M.; Thoma, Steven G.; Ashley, Carol S.; Reed, Scott T.

    2002-01-01

    A new class of composite zeolite membranes and synthesis techniques therefor has been invented. These membranes are essentially defect-free, and exhibit large levels of transmembrane flux and of chemical and isotopic selectivity.

  12. Cinzas de casca de arroz como fonte alternativa de silício para a síntese de zeólita beta

    OpenAIRE

    Enzweiler, Heveline; Coutinho, Elisa Barbosa; Schwaab, Marcio

    2014-01-01

    Rice husk ash is an agroindustrial residue generated in large scale that can cause environmental problems and risks to people health. As a solution to this problem, this ash could be used as an alternative source of high reactive silica, with a wide field of applications, such as, for example, in the synthesis of catalysts with high silicon content. In this work, beta zeolite was synthesized using amorphous silica, extracted from rice husk ash, and pseudo-boehmite. Using this alternative sour...

  13. Hydraulic conductivity of compacted zeolites.

    Science.gov (United States)

    Oren, A Hakan; Ozdamar, Tuğçe

    2013-06-01

    Hydraulic conductivities of compacted zeolites were investigated as a function of compaction water content and zeolite particle size. Initially, the compaction characteristics of zeolites were determined. The compaction test results showed that maximum dry unit weight (γ(dmax)) of fine zeolite was greater than that of granular zeolites. The γ(dmax) of compacted zeolites was between 1.01 and 1.17 Mg m(-3) and optimum water content (w(opt)) was between 38% and 53%. Regardless of zeolite particle size, compacted zeolites had low γ(dmax) and high w(opt) when compared with compacted natural soils. Then, hydraulic conductivity tests were run on compacted zeolites. The hydraulic conductivity values were within the range of 2.0 × 10(-3) cm s(-1) to 1.1 × 10(-7) cm s(-1). Hydraulic conductivity of all compacted zeolites decreased almost 50 times as the water content increased. It is noteworthy that hydraulic conductivity of compacted zeolite was strongly dependent on the zeolite particle size. The hydraulic conductivity decreased almost three orders of magnitude up to 39% fine content; then, it remained almost unchanged beyond 39%. Only one report was found in the literature on the hydraulic conductivity of compacted zeolite, which is in agreement with the findings of this study.

  14. Discovery of optimal zeolites for challenging separations and chemical transformations using predictive materials modeling

    Science.gov (United States)

    Bai, Peng; Jeon, Mi Young; Ren, Limin; Knight, Chris; Deem, Michael W.; Tsapatsis, Michael; Siepmann, J. Ilja

    2015-01-01

    Zeolites play numerous important roles in modern petroleum refineries and have the potential to advance the production of fuels and chemical feedstocks from renewable resources. The performance of a zeolite as separation medium and catalyst depends on its framework structure. To date, 213 framework types have been synthesized and >330,000 thermodynamically accessible zeolite structures have been predicted. Hence, identification of optimal zeolites for a given application from the large pool of candidate structures is attractive for accelerating the pace of materials discovery. Here we identify, through a large-scale, multi-step computational screening process, promising zeolite structures for two energy-related applications: the purification of ethanol from fermentation broths and the hydroisomerization of alkanes with 18-30 carbon atoms encountered in petroleum refining. These results demonstrate that predictive modelling and data-driven science can now be applied to solve some of the most challenging separation problems involving highly non-ideal mixtures and highly articulated compounds.

  15. Nanosized zeolites as a perspective material for conductometric biosensors creation

    Science.gov (United States)

    Kucherenko, Ivan; Soldatkin, Oleksandr; Kasap, Berna Ozansoy; Kirdeciler, Salih Kaan; Kurc, Burcu Akata; Jaffrezic-Renault, Nicole; Soldatkin, Alexei; Lagarde, Florence; Dzyadevych, Sergei

    2015-05-01

    In this work, the method of enzyme adsorption on different zeolites and mesoporous silica spheres (MSS) was investigated for the creation of conductometric biosensors. The conductometric transducers consisted of gold interdigitated electrodes were placed on the ceramic support. The transducers were modified with zeolites and MSS, and then the enzymes were adsorbed on the transducer surface. Different methods of zeolite attachment to the transducer surface were used; drop coating with heating to 200°C turned out to be the best one. Nanozeolites beta and L, zeolite L, MSS, and silicalite-1 (80 to 450 nm) were tested as the adsorbents for enzyme urease. The biosensors with all tested particles except zeolite L had good analytical characteristics. Silicalite-1 (450 nm) was also used for adsorption of glucose oxidase, acetylcholinesterase, and butyrylcholinesterase. The glucose and acetylcholine biosensors were successfully created, whereas butyrylcholinesterase was not adsorbed on silicalite-1. The enzyme adsorption on zeolites and MSS is simple, quick, well reproducible, does not require use of toxic compounds, and therefore can be recommended for the development of biosensors when these advantages are especially important.

  16. The kinetics of citral hydrogenation over Pd supported on clinoptilolite rich natural zeolite

    OpenAIRE

    Yılmaz, Selahattin; Uçar, Şule; Artok, Levent; Güleç, Hilal

    2005-01-01

    The liquid phase hydrogenation of citral has been investigated over Pd (2.42%) supported on clinoptilolite rich natural zeolite catalyst for different reaction conditions. The zeolite support did not affect the active metal properties. This was attributed to the large size of Pd particles on the support. High selectivity (90%) to citronellal was obtained at complete conversion of citral. The catalytic activity increased with reaction temperature (80, 100, 120°C) following an Arrhenius behavio...

  17. Fabrication and catalytic tests of MCM-22/silicon carbide structured catalysts.

    Science.gov (United States)

    Gu, Lijun; Ma, Ding; Hu, Gang; Wu, Jingjing; Wang, Hongxia; Sun, Changyong; Yao, Songdong; Shen, Wenjie; Bao, Xinhe

    2010-10-28

    The structured catalyst of zeolite MCM-22/silicon carbide (SiC) was prepared for the first time through the in situ hydrothermal synthesis approach. The zeolite loading of the structured catalyst could be tuned by changing the synthesis time and applying alkali pre-treatment of SiC substrate. An additional silica layer formed on SiC substrate after the precalcination treatment facilitated the crystallization of MCM-22 zeolite on the SiC substrate. The MCM-22/SiC structured catalyst thus prepared exhibited good catalytic performance in the methane dehydroaromatization reaction.

  18. Mesoporous zeolite single crystals for catalytic hydrocarbon conversion

    DEFF Research Database (Denmark)

    Schmidt, I.; Christensen, C.H.; Hasselriis, Peter

    2005-01-01

    Recently, mesoporous zeolite single crystals were discovered. They constitute a novel family of materials that features a combined micropore and mesopore architecture within each individual crystal. Here, we briefly summarize recent catalytic results from cracking and isomerization of alkalies......, alkylation of aromatics and present new results on isomerization of aromatics. Specifically, the shape-selective isomerization of meta-xylenc into para-xylene and ortho-xylene is studied. In all these reactions, rnesoporous zeolite single crystals prove to be unique catalysts since they provide easy...... transport to and from active sites and at the same time maintain the shape-selectivity required. Thus, all these results support the idea that the beneficial effect of the mesopores system in the mesoporous zeolite single crystals call be solely attributed to enhanced mass transport....

  19. Hydroconversion of n-alkanes on bifunctional zeolites with unusual pore architecture

    Energy Technology Data Exchange (ETDEWEB)

    Doerr, G.; Tontisirin, S.; Ernst, S. [Technische Univ. Kaiserslautern (Germany). Dept. of Chemistry, Chemical Technology

    2010-12-30

    Zeolites MCM-68 and ZSM-18, both possessing unusual pore architectures, were synthesized via hydrothermal synthesis using optimized methods. X-ray powder diffraction and scanning electron microscopy revealed that the obtained zeolites are well crystallized and do not contain visible amounts of amorphous material. The bifunctional forms of MCM- 68 and ZSM-18 (viz. the acid form loaded with small amounts of palladium) were characterized using the hydroconversion of n-decane as catalytic test reaction. In this reaction, both catalysts showed the typical behaviour known from other bifunctional large pore zeolites. (orig.)

  20. Idea of environmental catalyst and its application; Kankyo shokubai no hasso to sono riyo

    Energy Technology Data Exchange (ETDEWEB)

    Inumaru, K. [The University of Tokyo, Tokyo (Japan)

    1997-10-20

    The catalyst creating environmental conservation and comfortable environment is generally named an `environmental catalyst (EC).` EC is roughly classified into direct and indirect type ECs. Purification catalysts for automobile exhaust gas, and catalysts for chemical production process are under investigation as direct and indirect type ECs, respectively. The catalyst was found which can remove NOx under the coexistence of oxygen by using hydrocarbon as reductant. In addition, the practical exhaust gas purification catalyst was also developed for lean-burn engines by combining noble metal catalysts with NOx absorbing materials or zeolite superior in reductant adsorbing power. {epsilon}-caprolactam as raw material of nylon 6 is synthesized from cyclohexanoneoxime through Beckmann` rearrangement reaction. Zeolite system solid catalysts using no ammonia are under investigation. An environment-friendly synthesis method using not phosgene but catalyst was proposed for production of dimethyl carbonate. How to utilize catalysts for global material circulation remains unsolved for the future study. 5 refs.

  1. Diethyl Ether Production Process with Various Catalyst Type

    Directory of Open Access Journals (Sweden)

    Widayat

    2013-01-01

    Full Text Available Several H-zeolite and HZSM-5 catalysts was preparated and their characters have also been investigated. H-zeolit Catalyst was preparated from Natural Zeolite that obtained from Malang District and Gunung Kidul District. Diethyl ether was produced by Ethanol with concentration of 95%. This research use fixed bed reactor that 1 gram of catalyst as bed catalyst, atmospheric pressure and temperature 140oC as the operating condition. Ethanol vapor from vaporization tank was driven by 200 ml/min Nitrogen stream. The responds in this research is liquid product concentration; diethyl ether, ethanol, methanol and water concentration. The results showed that the largest ethanol conversion was produced by the use of 56.44% HZSM-5 and the largest yield of diethyl ether diethyl was produced by the use of alumina and H-zeolite catalyst. The larger ratio between natural zeolite with HCl solvent will produce the larger surface area of catalyst and ethanol conversion. The largest ethanol conversion was produced at reactan ratio 1:20.

  2. Synthesis of 3-(1-Cyclohexenyl)-2-butanone via Environmentally Friendly Catalysts

    Institute of Scientific and Technical Information of China (English)

    ZHAO Zhen-hua

    2003-01-01

    We substituted several environmentally friendly catalysts which included HY and H-β zeolites, various cation-exchanged β zeolites, and solid-supported ferric chloride for conventional catalysts for the synthesis of 3-(1-cyclohexenyl)-2-butanone from the reaction of ethylidenecyclohexane with acetic anhydride at room temperature. HY zeolite was found to be the most effective for this reaction, and gave the acylated product in a 72% yield under the conditions of n(ethylidenecyclohexane)/n(acetic anhydride)/m(HY zeolite)=1 mmol/10 mmol/0.100 g, reaction temperature 25 ℃ and reaction time 2 h. The used HY zeolite can be recovered, regenerated and gave almost the same yield as the fresh one. The lifetime of the HY zeolite is over 80 h. The effect of different factors on the reaction has also been investigated.

  3. Development and Application of CDOS Series Catalysts for Bottoms Cracking

    Institute of Scientific and Technical Information of China (English)

    Wang Mingjin; Xu Mingde; Zhu Yuxia

    2013-01-01

    Development of CDOS catalyst for bottoms cracking is based on DOSY zeolite, which is characterized by high metal tolerance. The results of DOSY tests have shown that the catalyst has better activity retention at high metal content in the feed. The performance of catalyst tested in the bench scale was superior over that of the reference catalyst. The results of catalyst application have shown that the CDOS series catalysts have better bottoms cracking activity, high metal tolerance, excellent dry gas selectivity, and enhanced liquid yield.

  4. Catalytic activity of zeolites in the formation of cresols from phenol and toluene

    Energy Technology Data Exchange (ETDEWEB)

    Kozhevnikov, S.A.; Sibarov, D.A.; Proskuryakov, V.A.

    1988-06-10

    This paper explores a synthetic method of obtaining cresols from phenol and toluene in order to replace coal tar with more abundant chemicals as raw materials for cresol synthesis. The method consists of the transmethylation of phenol with toluene under the action of zeolite catalysts. The zeolites tested include NaY, MgCaY, MnCaY, LiCaY, NiCaY, CrCaY, CaHY, and LaCaHY. Direct dependence of the activity of zeolite catalysts in transmethylation on the strength of the surface acidic centers was observed. Increased substitution of Ca divalent cations by La divalent cations promoted high activity and selectivity of the catalyst in formation of cresols.

  5. for zeolite coating

    Directory of Open Access Journals (Sweden)

    Carlos Renato Rambo

    2006-01-01

    Full Text Available Biotemplating is the processing of microcellular ceramics by reproduction of natural morphologies, where the microstructural features of the biotemplate are maintained in the biomorphic ceramic. Different biotemplates with distinct pore anatomies were used to produce biomorphic supports for the zeolite coating: wood, cardboard, sea-sponge and sisal. The biomorphic ceramics were produced by distinguished processing routes: Al-gas infiltration-reaction, liquid-metal infiltration, dip-coating and sol-gel synthesis, in order to produce nitrides, carbides and oxides, depending on the processing conditions. The zeolite coating was performed by hydrothermal growth of MFI-type (Silicalite-1 and ZSM-5 zeolite crystals onto the internal pore walls of the biomorphic templates. The final biomorphic ceramic-zeolite composites were physically characterized, evaluated in terms of their gas adsorption capabilities and correlated to their microstructure and specific pore anatomy. The combination of the properties of the biomorphic ceramics with the adsorption properties of zeolites results in materials with distinct properties as potential candidates for adsorption and catalytic applications due to their characteristic porosity, molecular sieving capabilities and high thermo-mechanical strength.

  6. Catalytic Dehydration of 4-Hydroxy-3-hexanone to 4-Hexen-3-one over HZSM-5 Zeolite

    Institute of Scientific and Technical Information of China (English)

    Huang Kai; Zheng Haitao; Tao Keyi

    2013-01-01

    A study on catalytic dehydration of 4-hydroxy-3-hexanone (HH) to 4-hexen-3-one (HO) was carried out through conversion of HH over HZSM-5 zeolite catalyst in a ifxed-bed reactor (FBR) operating under atmospheric pressure. The test indicated a relatively high activity of the HZSM-5 zeolite capable of achieving a HH conversion of 99.2% and a HO yield of 83.5%. Catalyst deactivation could be prevented by increasing the reaction temperature by 10℃ for every 20 h and adding 2.0% of piperidine in the feed. A catalyst stability test (for 100 h) in FBR showed that the catalyst was active even after 100 h of time-on-stream with HH conversion remaining at 99.2% and HO yield still reaching over 83.5%. Regenera-tion experiment showed that the regenerated catalyst demonstrated a catalytic performance comparable to the fresh one.

  7. Ru complexes of Hoveyda-Grubbs type immobilized on lamellar zeolites: activity in olefin metathesis reactions.

    Science.gov (United States)

    Balcar, Hynek; Žilková, Naděžda; Kubů, Martin; Mazur, Michal; Bastl, Zdeněk; Čejka, Jiří

    2015-01-01

    Hoveyda-Grubbs type catalysts with cationic tags on NHC ligands were linker-free immobilized on the surface of lamellar zeolitic supports (MCM-22, MCM-56, MCM-36) and on mesoporous molecular sieves SBA-15. The activity of prepared hybrid catalysts was tested in olefin metathesis reactions: the activity in ring-closing metathesis of citronellene and N,N-diallyltrifluoroacetamide decreased in the order of support MCM-22 ≈ MCM-56 > SBA-15 > MCM-36; the hybrid catalyst based on SBA-15 was found the most active in self-metathesis of methyl oleate. All catalysts were reusable and exhibited low Ru leaching (<1% of Ru content). XPS analysis revealed that during immobilization ion exchange between Hoveyda-Grubbs type catalyst and zeolitic support occurred in the case of Cl(-) counter anion; in contrast, PF6 (-) counter anion underwent partial decomposition.

  8. Ru complexes of Hoveyda–Grubbs type immobilized on lamellar zeolites: activity in olefin metathesis reactions

    Science.gov (United States)

    Žilková, Naděžda; Kubů, Martin; Mazur, Michal; Bastl, Zdeněk; Čejka, Jiří

    2015-01-01

    Summary Hoveyda–Grubbs type catalysts with cationic tags on NHC ligands were linker-free immobilized on the surface of lamellar zeolitic supports (MCM-22, MCM-56, MCM-36) and on mesoporous molecular sieves SBA-15. The activity of prepared hybrid catalysts was tested in olefin metathesis reactions: the activity in ring-closing metathesis of citronellene and N,N-diallyltrifluoroacetamide decreased in the order of support MCM-22 ≈ MCM-56 > SBA-15 > MCM-36; the hybrid catalyst based on SBA-15 was found the most active in self-metathesis of methyl oleate. All catalysts were reusable and exhibited low Ru leaching (<1% of Ru content). XPS analysis revealed that during immobilization ion exchange between Hoveyda–Grubbs type catalyst and zeolitic support occurred in the case of Cl− counter anion; in contrast, PF6 − counter anion underwent partial decomposition. PMID:26664629

  9. Synthesis of Zeolites Using the ADOR (Assembly-Disassembly-Organization-Reassembly) Route.

    Science.gov (United States)

    Wheatley, Paul S; Čejka, Jiří; Morris, Russell E

    2016-04-03

    Zeolites are an important class of materials that have wide ranging applications such as heterogeneous catalysts and adsorbents which are dependent on their framework topology. For new applications or improvements to existing ones, new zeolites with novel pore systems are desirable. We demonstrate a method for the synthesis of novel zeolites using the ADOR route. ADOR is an acronym for Assembly, Disassembly, Organization and Reassembly. This synthetic route takes advantage of the assembly of a relatively poorly stable that which can be selectively disassembled into a layered material. The resulting layered intermediate can then be organized in different manners by careful chemical manipulation and then reassembled into zeolites with new topologies. By carefully controlling the organization step of the synthetic pathway, new zeolites with never before seen topologies are capable of being synthesized. The structures of these new zeolites are confirmed using powder X-ray diffraction and further characterized by nitrogen adsorption and scanning electron microscopy. This new synthetic pathway for zeolites demonstrates its capability to produce novel frameworks that have never been prepared by traditional zeolite synthesis techniques.

  10. Fluorescence labelling as tool for zeolite particle tracking in nanoremediation approaches

    Energy Technology Data Exchange (ETDEWEB)

    Gillies, Glenn; Mackenzie, Katrin; Kopinke, Frank-Dieter; Georgi, Anett

    2016-04-15

    Colloidal Fe-zeolites such as Fe-BEA-35 are currently under study as new adsorbent and catalyst materials for in-situ chemical oxidation with H{sub 2}O{sub 2}. As for nanoremediation in general, the availability of suitable particle detection methods is a requirement for successful process development and particle tracing. Detection and distinguishing between natural colloids and introduced particles with a similar composition are a challenge. By means of fluorescence labelling, a highly specific detection option for Fe-BEA-35 was developed. ‘Ship-in-a-bottle’ synthesis of fluorescein within the zeolite pores, which was applied for the first time for a BEA type zeolite, provides a product with stable and non-extractable fluorescence. When the fluorescent labelled zeolite is added at a concentration of 1 wt.% referring to the total zeolite mass, a very low detection limit of 1 mg/L of total zeolite is obtained. Compared to commonly applied turbidity measurements, detection via fluorescence labelling is much more specific and sensitive. Fluorescence is only marginally affected by carboxymethyl cellulose, which is frequently applied as stabilizer in application suspensions but will be depleted upon contact with H{sub 2}O{sub 2}. Transport properties of fluorescent labelled and non-labelled Fe-zeolite particles are in agreement as determined in a column study with quartz sand and synthetic groundwater (classified as very hard). - Highlights: • Fluorescent BEA zeolite was prepared for first time by ‘ship-in-a-bottle’ synthesis. • Fluorescein synthesized inside zeolite channels is stable and non-extractable. • Detection limit of Fe-zeolite particles in suspension with 1 wt.% fluorescent zeolite is 1 mg/L. • Transport properties of fluorescent and Fe-loaded BEA particles are identical.

  11. Thiophene hydrodesulfurization over CoMo/Al2O3-CuY catalysts: Temperature effect study

    Directory of Open Access Journals (Sweden)

    Yamina Boukoberine

    2016-09-01

    Full Text Available CoMo/γ-Al2O3-CuY catalysts are prepared by physically mixing CoMo/γ-Al2O3 catalyst with Cu-exchanged Y zeolite. The CuY zeolite is prepared by the solid state ion exchange technique. The thiophene hydrodesulfurization is performed in a fixed bed reactor at high temperature and atmospheric pressure. The results show that the presence of CuY zeolite particles in CoMo/Al2O3 catalyst can have a noticeable effect on both the conversion and product selectivities. An increasing zeolite loading in catalyst results in a decrease of the thiophene HDS activity. This decrease is probably caused by the formation of heavy compounds and the deactivation of the zeolite at high temperatures.

  12. Production of high quality gasoline from waste polyethylene derived heavy oil over Ni-REY catalyst in steam atmosphere

    Energy Technology Data Exchange (ETDEWEB)

    Masuda, Takao; Kuwahara, Hiroshi; Mukai, Shin; Hashimoto, Kenji [Kyoto University Honnmachi (Japan). Graduate School of Engineering

    1999-07-01

    Nickel and rare earth metal exchanged Y-type zeolite catalyst (Ni-REY) was prepared for producing light fuels (gasoline and kerosene) by the catalytic cracking of heavy oil from waste plastics in a steam atmosphere. The Ni in the catalyst was found to exhibit catalysis for transportation of hydrogen atoms from steam to hydrocarbons. In a steam atmosphere, strong acid sites of the catalyst, which usually cause excessive cracking, were covered with steam molecules, leading to a high yield of liquid fuels. Experiments using MFI zeolite in a nitrogen atmosphere were also conducted for comparison. During the repetition of sequences of reaction and regeneration of the catalysts, MFI zeolite was gradually deactivated, whereas NI-REY was found to show constant activity. Furthermore, the selectivity towards gasoline was higher than MFI zeolite (NI-REY in steam: 78%, MFI type zeolite in N{sub 2} 35%). (author)

  13. Synthesis of zeolite membranes

    Institute of Scientific and Technical Information of China (English)

    JIANG Haiyang; ZHANG Baoquan; Y. S. Lin; LI Yongdan

    2004-01-01

    Zeolite membranes offer great application potentials in membrane separation and/or reaction due to their excellent separation performance and catalytic ability. Up to present, various synthesis methods of zeolite membranes have been developed, including embedded method,in-situ hydrothermal synthesis method, and secondary growth method etc. Compared with the in-situ hydrothermal synthesis method, the secondary growth method possesses a variety of advantages such as easier operation, higher controllability in crystal orientation, microstructure and film thickness, leading to much better reproducibility. This review provides a concise summary and analysis of various synthesis methods reported in the literature. In particular, the secondary growth method was discussed in detail in terms of crystal orientation, defects and crystal grain layers. Some critical issues were also highlighted, which were conducive to the improvement in the synthesis technology of zeolite membranes.

  14. Advances in nanosized zeolites

    Science.gov (United States)

    Mintova, Svetlana; Gilson, Jean-Pierre; Valtchev, Valentin

    2013-07-01

    This review highlights recent developments in the synthesis of nanosized zeolites. The strategies available for their preparation (organic-template assisted, organic-template free, and alternative procedures) are discussed. Major breakthroughs achieved by the so-called zeolite crystal engineering and encompass items such as mastering and using the physicochemical properties of the precursor synthesis gel/suspension, optimizing the use of silicon and aluminium precursor sources, the rational use of organic templates and structure-directing inorganic cations, and careful adjustment of synthesis conditions (temperature, pressure, time, heating processes from conventional to microwave and sonication) are addressed. An on-going broad and deep fundamental understanding of the crystallization process, explaining the influence of all variables of this complex set of reactions, underpins an even more rational design of nanosized zeolites with exceptional properties. Finally, the advantages and limitations of these methods are addressed with particular attention to their industrial prospects and utilization in existing and advanced applications.

  15. Catalytic activities of zeolite compounds for decomposing aqueous ozone.

    Science.gov (United States)

    Kusuda, Ai; Kitayama, Mikito; Ohta, Yoshio

    2013-12-01

    The advanced oxidation process (AOP), chemical oxidation using aqueous ozone in the presence of appropriate catalysts to generate highly reactive oxygen species, offers an attractive option for removing poorly biodegradable pollutants. Using the commercial zeolite powders with various Si/Al ratios and crystal structures, their catalytic activities for decomposing aqueous ozone were evaluated by continuously flowing ozone to water containing the zeolite powders. The hydrophilic zeolites (low Si/Al ratio) with alkali cations in the crystal structures were found to possess high catalytic activity for decomposing aqueous ozone. The hydrophobic zeolite compounds (high Si/Al ratio) were found to absorb ozone very well, but to have no catalytic activity for decomposing aqueous ozone. Their catalytic activities were also evaluated by using the fixed bed column method. When alkali cations were removed by acid rinsing or substituted by alkali-earth cations, the catalytic activities was significantly deteriorated. These results suggest that the metal cations on the crystal surface of the hydrophilic zeolite would play a key role for catalytic activity for decomposing aqueous ozone.

  16. 多级结构ZSM-5沸石分子筛的合成及其Mo基催化剂在甲烷无氧脱氢芳构化中的应用%Synthesis of Hierarchical ZSM-5 Zeolite and Performance of Its Mo-Based Catalyst for Methane Dehydroaromatization

    Institute of Scientific and Technical Information of China (English)

    于素霞; 杨建华; 初乃波; 李刚; 鲁金明; 王金渠

    2009-01-01

    A hierarchical spherical-like ZSM-5 zeolite was synthesized using multiwall carbon nanotubes as secondary template. First, the nanotubes were purified by reflux with concentrated hydrochloric acid for 24 h. This purification step was repeated until the hydrochloric acid was no longer colored by impurities from the nanotubes (typically 3-4 times). Then the disposed nanotubes were added into the synthesis solution of ZSM-5, which was obtained by mixing H_2O, tetraethylorthosilicate, Al(C_3H_8O)_3, and tetrapropylammonium hydroxide (TPAOH). Afterward, this mixture was subjected to crystallization at varying temperatures. The obtained products were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and nitrogen adsorption analysis. The results indicated that ZSM-5 zeolite with uniform size of 300-400 nm was synthesized, and it was spherical-like aggregates and has hierarchical structure constructed by many ZSM-5 nanotubes of 20-40 nm. The hierarchical ZSM-5 zeolite was modified to form a Mo/HZSM-5 catalyst, and its catalytic performance for methane dehydroaromatization was investigated. The modified Mo/HZSM-5 catalyst exhibited CH_4 conversion as high as 19% and better life time. The CH_4 conversion was kept at 10% even when the reaction time was 24 h. It is suggested that hierarchical structure was favorable for the enhancement of catalyst performance, which is due to the presence of both micropores and mesopores.%以经盐酸预处理的碳纳米管为第二模板,在不添加其它有机溶剂的情况下,仅通过控制晶化条件,即采用变温水热晶化法合成具有多级结构的ZSM-5分子筛.通过x射线衍射、红外光谱测试、透射电镜和N2吸附对合成的分子筛进行了表征,结果表明,该合成分子筛呈近球形,是由纳米棒自组装形成的具有多级结构的亚微米球.该分子筛改性后用于甲烷无氧脱氢芳构化反应,显示出良好的催化性能,

  17. The growth of zeolites A, X and mordenite in space

    Science.gov (United States)

    Sacco, Albert, Jr.; Bac, N.; Coker, E. N.; Dixon, A. G.; Warzywoda, J.; Thompson, R. W.

    1994-01-01

    Zeolites are a class of crystalline aluminosilicate materials that form the backbone of the chemical process industry worldwide. They are used primarily as adsorbents and catalysts and support to a significant extent the positive balance of trade realized by the chemical industry in the United States (around $19 billion in 1991). The magnitude of their efforts can be appreciated when one realizes that since their introduction as 'cracking catalysts' in the early 1960's, they have saved the equivalent of 60 percent of the total oil production from Alaska's North Slope. Thus the performance of zeolite catalysts can have a profound effect on the U.S. economy. It is estimated that a 1 percent increase in yield of the gasoline fraction per barrel of oil would represent a savings of 22 million barrels of crude oil per year, representing a reduction of $400 million in the United States' balance of payments. Thus any activity that results in improvement in zeolite catalyst performance is of significant scientific and industrial interest. In addition, due to their 'stability,' uniformity, and, within limits, their 'engineerable' structures, zeolites are being tested as potential adsorbents to purify gases and liquids at the parts-per-billion levels needed in today's electronic, biomedical, and biotechnology industries and for the environment. Other exotic applications, such as host materials for quantum-confined semiconductor atomic arrays, are also being investigated. Because of the importance of this class of material, extensive efforts have been made to characterize their structures and to understand their nucleation and growth mechanisms, so as to be able to custom-make zeolites for a desired application. To date, both the nucleation mechanics and chemistry (such as what are the 'key' nutrients) are, as yet, still unknown for many, if not all, systems. The problem is compounded because there is usually a 'gel' phase present that is assumed to control the degree of

  18. 过渡金属基分子筛SCR催化剂失活机制及抗失活技术研究进展%Research Progress on Deactivation and Resistance of Transitional Metal Based Zeolite SCR Catalysts

    Institute of Scientific and Technical Information of China (English)

    马静; 翁端; 吴晓东; 司知蠢

    2011-01-01

    过渡金属基分子筛是在氨选择性催化还原氮氧化物技术领域广泛应用的一类催化材料,在实际应用中容易中毒失活.失活形式主要有水热老化失活,P、S中毒失活,HCs中毒失活及尿素中毒失活等.本文分析了过渡金属基分子筛催化剂的4种失活机制及相应的抗失活工艺,并展望了过渡金属基分子筛的发展方向.%Transitional metal based zeolites are widely used to remove nitrogen oxides by NH3-SCR, which will eventually become de-activated in practical application proceses, including hydrothermal aging, P and S poisoning, HCs poisoning and urea poisoning. The deactivation mechanisms and the related methods to improve the resistance to deactivation are reviewed. The development trends of the transitional metal based zeolite are outlined.

  19. Structure-activity relations for Ni-containing zeolites during NO reduction II. Role of the chemical state of Ni

    NARCIS (Netherlands)

    Mosqueda-Jiménez, B.I.; Jentys, A.; Seshan, K.; 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 fra

  20. High Yield of Liquid Range Olefins Obtained by Converting i-Propanol over Zeolite H-ZSM-5

    DEFF Research Database (Denmark)

    Mentzel, Uffe Vie; Shunmugavel, Saravanamurugan; Hruby, S.L.;

    2009-01-01

    Methanol, ethanol, and i-propanol were converted under methanol-to-gasoline (MTH)-like conditions (400 degrees C, 1-20 bar) over zeolite H-ZSM-5. For methanol and ethanol, the catalyst lifetimes and conversion capacities are comparable, but when i-propanol is used as the reactant, the catalyst li...

  1. Rapid synthesis of an aluminum-rich MSE-type zeolite by the hydrothermal conversion of an FAU-type zeolite.

    Science.gov (United States)

    Inagaki, Satoshi; Tsuboi, Yasuyuki; Nishita, Yuji; Syahylah, Tuan; Wakihara, Toru; Kubota, Yoshihiro

    2013-06-10

    An aluminum-rich MSE-type zeolite (Si/Al is as small as 7) has been successfully synthesized in a remarkably short crystallization period of only 3 days by the hydrothermal conversion of an FAU-type zeolite, presumably by the assembly of four-membered-ring (4-R) aluminosilicate oligomers supplied by the double 6-R (D6R) components of the FAU framework with the aid of the structure-directing agents and seed crystals. The dealuminated version of the aluminum-rich MSE-type zeolite showed a high level of coke durability in addition to a significant yield of propylene, which indicates that this novel zeolitic material is suitable for industrial applications as a highly selective and long-lived catalyst.

  2. Rhenium Nanochemistry for Catalyst Preparation

    Directory of Open Access Journals (Sweden)

    Vadim G. Kessler

    2012-08-01

    Full Text Available The review presents synthetic approaches to modern rhenium-based catalysts. Creation of an active center is considered as a process of obtaining a nanoparticle or a molecule, immobilized within a matrix of the substrate. Selective chemical routes to preparation of particles of rhenium alloys, rhenium oxides and the molecules of alkyltrioxorhenium, and their insertion into porous structure of zeolites, ordered mesoporous MCM matrices, anodic mesoporous alumina, and porous transition metal oxides are considered. Structure-property relationships are traced for these catalysts in relation to such processes as alkylation and isomerization, olefin metathesis, selective oxidation of olefins, methanol to formaldehyde conversion, etc.

  3. 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.

  4. Study on Removing Trace Olefins in Aromatic Hydrocarbons with HPMo-loaded Y Zeolites

    Institute of Scientific and Technical Information of China (English)

    Jiang Zhenghong; Zeng Haiping; Shi Li

    2008-01-01

    HPMo-loaded Y-zeolites were prepared for the removal of trace olefins from aromatic hydrocarbons.The temperature of calcination and the proportion of phospho-molybdic acid in the catalyst were studied. The catalytic activity for olefins removal and the service life of the catalyst were tested in a fixed bed microreactor. The results showed that the catalyst containing 3% phospho-molybdic acid, which was calcined at 550℃,demonstrated the best activity for olefins removal. The catalyst could be regenerated and could perform still very well. Catalyst characterization was performed by XRD and measured by pyridine-FTIR spectrometry. The test results indicated that the activity of the catalyst was related with the effect of acid concentration and acid strength. Besides, the deactivation of the catalyst was associated with the formation of coke deposits and the deactivated catalyst could recover its activity by oxidation with air under a proper temperature.

  5. Zeolites and Catalysis

    Science.gov (United States)

    1999-12-15

    Handbook of Heterogeneous Catalysis ,Vol. als: State of the Art 1994, Studies in Surface Science and 5, Wiley-VCH, Weinheim, 1997, p. 2329. Catalysis, Vol...Weitkamp (Eds.), in Zeolite and Microporous Materials, Studies in Surface Handbook of Heterogeneous Catalysis , Vol. 4, Wiley-VCH, Science and Catalysis

  6. Influence of zeolitic structure on photoreduction property and hydrogen evolution reaction

    Energy Technology Data Exchange (ETDEWEB)

    Chatti, Ravikrishna V.; Dubey, Nidhi; Joshi, Meenal V.; Labhsetwar, Nitin K.; Rayalu, Sadhana S. [National Environmental Engineering Research Institute (NEERI-CSIR), Environmental Materials Unit, Nehru Marg, 440020 Nagpur, Maharashtra (India); Joshi, P.N. [National Chemical Laboratory (NCL-CSIR), Pune (India)

    2010-03-15

    A new photocatalytic material developed by supporting TiO{sub 2} in combination with transition metal ion like cobalt and heteropolyacid (HPA) on the surface is facilitating enhanced photoreduction of water and methyl orange. Zeolites being a solid acid play an important role in the electron transfer reaction, facilitated by the Lewis acid sites in the form of aluminium ions. In the present work, four different zeolite matrices namely, NaY zeolite, ultrastable zeolite Y, beta zeolite and titanium silicate-1 have been used for the synthesis of new photocatalytic materials. These materials have been evaluated for water splitting by an initial screening procedure using methyl orange photoreduction. The photocatalyst containing Na Y has emerged as a potential photocatalyst with hydrogen evolution rate of 2730 {mu}mol/h/g of TiO{sub 2}. Hydrogen evolution was not observed for the composite photocatalysts synthesized using the other zeolite matrices. It has been observed that physico-chemical properties like Si/Al ratio, acidity and basicity of the zeolite support have a tremendous influence on the photoreduction property of these zeolite matrices. (author)

  7. FAU分子筛封装Co(Salen)配合物复合催化剂的制备及其对氧还原电催化活性的研究%Study on preparation and electrocatalytic activity of Faujasite Zeolites encapsulated Co(Salen) complex catalysts on oxygen reduction

    Institute of Scientific and Technical Information of China (English)

    马飞; 张晶; 王文洋; 李瑞丰; 张蓉

    2013-01-01

    Zeolite Y,X and LSX encapsulated Co(Salen) complexes ( Co ( Salen)/Z) are prepared by flexible ligand method and characterized by FT-IR,UV-vis DRS and XRD. With these hybrid catalysts as modifier, the zeolite modified glassy carbon electrodes( Co( Salen)/Z( Z = Y,X, LSX)/GCE) are prepared by zeolite/polymer step-by-step coating and shows good electro-catalytical activity on oxygen reduction ( ORR). The electrochemical behavior and electro-catalytic activities of the Co(Salen)/Z(Z = Y,X, LSX)/GCE are studied using cyclic voltammetry (CV) in pH 6.86 buffer solution. The results show that it is Co( Salen) not Co2+ that is the electrocatalytic active centre of ORR in the pH 6. 86 buffer solution. The ratio of SiO2 :Al2 O3 of zeolites encapsulating Co (Salen) complex is of great influence on their electrocatalytic activity of Co(Salen) . The higher ratio of SiO2: A12O3 ,the better the electrocatalytic activity. The order of their electrocatalytic activity: Co( Salen)/LSX < Co( Salen)/X < Co( Salen)/Y.%运用自由配体法制备了不同硅铝比的FAU沸石分子筛(记作Z:包括高硅Y型、13X型和低硅X型(LSX))封装Co(Salen)配合物的复合材料,FTIR、UV-vis DRS、XRD表征表明配合物Co(Salen)被植入分子筛中形成复合催化剂(记作:Co(Salen)/Z).采用分子筛/聚合物分步涂覆法制备了固载Co(Salen)的分子筛修饰电极(记作:Co(Salen)/Z(Z=Y,X,LSX)/GCE).以循环伏安法(CV)研究了Co(Salen)/Z(Z=Y,X,LSX)/GCE修饰电极的电化学行为和电催化氧还原的催化活性.结果表明,Co(Salen)/Z(Z=Y,X,LSX)/GCE修饰电极电催化氧还原(ORR)的催化活性成分是Co(Salen),而且该Co(Salen)配合物对ORR的电催化活性受载体沸石分子筛骨架硅铝比的影响较大.对于硅铝比分别是2.O、2.5和5.8的LSX、X、Y型沸石分子筛而言,由硅铝较大的NaY所合成的电催化剂Co(Salen)/Y/GCF催化活性最高,且他们的电催化活性顺序为:Co(Salen)/Y> Co(Salen)/X> Co(Salen)/LSX.

  8. Zeolite crystal growth in space

    Science.gov (United States)

    Sacco, Albert, Jr.; Thompson, Robert W.; Dixon, Anthony G.

    1991-01-01

    The growth of large, uniform zeolite crystals in high yield in space can have a major impact on the chemical process industry. Large zeolite crystals will be used to improve basic understanding of adsorption and catalytic mechanisms, and to make zeolite membranes. To grow large zeolites in microgravity, it is necessary to control the nucleation event and fluid motion, and to enhance nutrient transfer. Data is presented that suggests nucleation can be controlled using chemical compounds (e.g., Triethanolamine, for zeolite A), while not adversely effecting growth rate. A three-zone furnace has been designed to perform multiple syntheses concurrently. The operating range of the furnace is 295 K to 473 K. Teflon-lined autoclaves (10 ml liquid volume) have been designed to minimize contamination, reduce wall nucleation, and control mixing of pre-gel solutions on orbit. Zeolite synthesis experiments will be performed on USML-1 in 1992.

  9. Modificação de zeólitas para uso em catálise Modifying zeolites for use in catalysis

    Directory of Open Access Journals (Sweden)

    Fernando J. Luna

    2001-12-01

    Full Text Available The use of zeolites and other molecular sieves as catalysts is discussed at an introductory level. The text includes a brief historic background on the use of zeolites in catalysis, and a discussion of some chemical and physical properties of silicalite, aluminosilicate, and aluminophosphate molecular sieves. The strategies currently used to chemically modify zeolites and related materials to produce catalysts with increased activity and selectivity are discussed, including the use of redox molecular sieves for hydrocarbon oxidation and the leaching of the active metals from the support.

  10. Synthesis and characterization of mesoporous hydrocracking catalysts

    Science.gov (United States)

    Munir, D.; Usman, M. R.

    2016-08-01

    Mesoporous catalysts have shown great prospective for catalytic reactions due to their high surface area that aids better distribution of impregnated metal. They have been found to contain more adsorption sites and controlled pore diameter. Hydrocracking, in the presence of mesoporous catalyst is considered more efficient and higher conversion of larger molecules is observed as compared to the cracking reactions in smaller microporous cavities of traditional zeolites. In the present study, a number of silica-alumina based mesoporous catalysts are synthesized in the laboratory. The concentration and type of surfactants and quantities of silica and alumina sources are the variables studied in the preparation of catalyst supports. The supports prepared are well characterized using SEM, EDX, and N2-BET techniques. Finally, the catalysts are tested in a high pressure autoclave reactor to study the activity and selectivity of the catalysts for the hydrocracking of a model mixture of plastics comprising of LDPE, HDPE, PP, and PS.

  11. Cu and Co exchanged ZSM-5 zeolites: activity towards no reduction and hydrocarbon oxidation

    Directory of Open Access Journals (Sweden)

    Martins Leandro

    2006-01-01

    Full Text Available |Cu x|[Si yAl]-MFI and |Co x|[Si yAl]-MFI catalysts were prepared by ion exchange from |Na|[Si yAl]-MFI zeolites (y = 12, 25 and 45. The activity of the catalysts was evaluated in the reduction of NO to N2 in an oxidative atmosphere using propane or methane as reducing agents. The Cu catalysts were only active with propane and they presented higher activity than the Co-based catalysts, the latter being active with both hydrocarbons. H2-TPR and DRS-UV/Vis data allowed correlation between the activity towards NO reduction and the presence of cationic charge-compensating species in the zeolite. It was also verified that the hydrocarbons are preferentially oxidised by O2, a reaction that occurs simultaneously with their oxidation with NO.

  12. Adsorption and photocatalytic degradation of pharmaceuticals and pesticides by carbon doped-TiO2 coated on zeolites under solar light irradiation.

    Science.gov (United States)

    An, Ye; de Ridder, David Johannes; Zhao, Chun; Schoutteten, Klaas; Bussche, Julie Vanden; Zheng, Huaili; Chen, Gang; Vanhaecke, Lynn

    2016-01-01

    To evaluate the performance of zeolite-supported carbon-doped TiO(2) composite catalysts toward target pollutants under solar light irradiation, the adsorption and photocatalytic degradation of 18 pharmaceuticals and pesticides with distinguishing features (molecular size and volume, and photolysis) were investigated using mordenite zeolites with SiO(2)/Al(2)O(3) ratios of 18 and 240. Different quantities of carbon-doped TiO(2) were coated on the zeolites, and then the finished composite catalysts were tested in demineralized, surface, and hospital wastewater samples, respectively. The composite photocatalysts were characterized by X-ray diffraction, field emission scanning electron microscopy, and surface area and porosity analyses. Results showed that a dispersed layer of carbon-doped TiO(2) is formed on the zeolite surface; this layer blocks the micropores of zeolites and reduces their surface area. However, these reductions did not significantly affect adsorption onto the zeolites. Our results demonstrated that zeolite-supported carbon-doped TiO(2) systems can effectively degrade 18 pharmaceuticals and pesticides in demineralized water under natural and simulated solar light irradiation. In surface and hospital wastewaters, zeolite-supported carbon-doped TiO(2) systems present excellent anti-interference capability against radical scavengers and competitive organics for pollutants removal, and higher pollutants adsorption on zeolites evidently enhances the removal rate of target pollutants in surface and hospital wastewater samples with a complicated matrix.

  13. Catalytic Flash Pyrolysis of Biomass Using Different Types of Zeolite and Online Vapor Fractionation

    KAUST Repository

    Imran, Ali

    2016-03-11

    Bio-oil produced from conventional flash pyrolysis has poor quality and requires expensive upgrading before it can be used as a transportation fuel. In this work, a high quality bio-oil has been produced using a novel approach where flash pyrolysis, catalysis and fractionation of pyrolysis vapors using two stage condensation are combined in a single process unit. A bench scale unit of 1 kg/h feedstock capacity is used for catalytic pyrolysis in an entrained down-flow reactor system equipped with two-staged condensation of the pyrolysis vapor. Zeolite-based catalysts are investigated to study the effect of varying acidities of faujasite Y zeolites, zeolite structures (ZSM5), different catalyst to biomass ratios and different catalytic pyrolysis temperatures. Low catalyst/biomass ratios did not show any significant improvements in the bio-oil quality, while high catalyst/biomass ratios showed an effective deoxygenation of the bio-oil. The application of zeolites decreased the organic liquid yield due to the increased production of non-condensables, primarily hydrocarbons. The catalytically produced bio-oil was less viscous and zeolites were effective at cracking heavy molecular weight compounds in the bio-oil. Acidic zeolites, H-Y and H-ZSM5, increased the desirable chemical compounds in the bio-oil such as phenols, furans and hydrocarbon, and reduced the undesired compounds such as acids. On the other hand reducing the acidity of zeolites reduced some of the undesired compounds in the bio-oil such as ketones and aldehydes. The performance of H-Y was superior to that of the rest of zeolites studied: bio-oil of high chemical and calorific value was produced with a high organic liquid yield and low oxygen content. H-ZSM5 was a close competitor to H-Y in performance but with a lower yield of bio-oil. Online fractionation of catalytic pyrolysis vapors was employed by controlling the condenser temperature and proved to be a successful process parameter to tailor the

  14. Hierarchical zeolites: Enhanced utilisation of microporous crystals in catalysis by advances in materials design

    DEFF Research Database (Denmark)

    Perez-Ramirez, Javier; Christensen, Claus H.; Egeblad, Kresten

    2008-01-01

    The introduction of synthetic zeolites has led to a paradigm shift in catalysis, separations, and adsorption processes, due to their unique properties such as crystallinity, high-surface area, acidity, ion-exchange capacity, and shape-selective character. However, the sole presence of micropores...... in these materials often imposes intracrystalline diffusion limitations, rendering low utilisation of the zeolite active volume in catalysed reactions. This critical review examines recent advances in the rapidly evolving area of zeolites with improved accessibility and molecular transport. Strategies to enhance...... catalyst effectiveness essentially comprise the synthesis of zeolites with wide pores and/or with short diffusion length. Available approaches are reviewed according to the principle, versatility, effectiveness, and degree of reality for practical implementation, establishing a firm link between...

  15. Trimethylamine as a probe molecule to differentiate acid sites in Y-FAU zeolite: FTIR study.

    Science.gov (United States)

    Sarria, Francisca Romero; Blasin-Aubé, Vanessa; Saussey, Jacques; Marie, Olivier; Daturi, Marco

    2006-07-06

    In heterogeneous catalysis acidity has a very important influence on activity and selectivity: correct determination of acidic properties is a base to improve industrial processes. The aim of this work was to study trimethylamine (TMA) as a probe molecule able to distinguish between the different Brønsted acid sites in zeolitic frameworks. Our work mainly focused on faujasite-type zeolites because the HY zeolite is one of the most used acidic catalysts in industrial processes. In this paper, typical IR bands assigned to TMA-protonated species (formed in supercages) are detected in the HY zeolite. TMA interacting by hydrogen bonding with the acid sites located in the sodalite units is also observed. The wavenumbers of some typical IR bands assigned to TMA-protonated species appear to depend on the acidic strength, and a complementary study with ZSM-5 and X-FAU samples confirms this proposition.

  16. Structural characteristics of zeolite/TiO2 composite and photocatalysis of toluene degradation

    Institute of Scientific and Technical Information of China (English)

    MING Caibing; WU Pingxiao

    2005-01-01

    Zeolite/TiO2 composite photocatalysts were prepared by adding a certain amount of mordenite in TiO2, and degradation experiments on toluene through photocatalytic reactions were implemented. In this paper, these photocatalysts were characterized by using SEM, IR, RAMAN, XRD and UV-Vis to shed light on the microstructure and photocatalytic performance of the composite photocatalysts. The results indicated that the structural hydroxy of zeolite can participate in bonding reaction with TiO2, the addition of zeolite can greatly reduce the diameter of nanometer TiO2 particles in the composite photocatalysts, and enhance the ultraviolet light absorptance of the composite photocatalysts. When the percentage content of zeolite reached 20%, the photocatalytic performance of this catalyst would be highest, with the toluene conversion rate up to 94.58%.

  17. Synthesis of ZSM-5 zeolite from lignite fly ash and rice husk ash

    Energy Technology Data Exchange (ETDEWEB)

    Chareonpanich, Metta; Namto, Teerapong; Kongkachuichay, Paisan [Department of Chemical Engineering, Kasetsart University, 50 Paholyothin Rd., Chatuchak, Bangkok 10900 (Thailand); Limtrakul, Jumras [Department of Chemistry, Kasetsart University, Chatuchak, Bangkok 10900 (Thailand)

    2004-10-15

    The lignite fly ash from the Mae-Moh power plant, Thailand, and rice husk ash were used as raw materials for ZSM-5 zeolite synthesis. Factors affecting the yield of ZSM-5 zeolite synthesized from fly ash, i.e., the SiO{sub 2}/Al{sub 2}O{sub 3} mole ratio, the presence of tetrapropyl ammonium bromide (TPABr, the structure-directing material for ZSM-5 zeolite synthesis), the holding temperature and time, and the initial pressure were investigated. It was found that without TPABr only zeolite P could be synthesized at SiO{sub 2}/Al{sub 2}O{sub 3} mole ratios of 2.8-200. In order to synthesize ZSM-5 zeolite, sodium silicate solution was added to adjust the SiO{sub 2}/Al{sub 2}O{sub 3} mole ratio in raw ash. The yield of ZSM-5 zeolite was as high as 59 wt.% when following conditions were used: SiO{sub 2}/Al{sub 2}O{sub 3} mole ratio, 40; the holding temperature, 210 C; the holding time, 4 h and the initial pressure, 4 bar. The catalytic performance for CO{sub 2} hydrogenation reaction of the ZSM-5 zeolite was preliminary tested and compared with that of commercial one. It was observed that there was no significant difference in the catalytic performance between these two catalysts.

  18. A Hierarchically Micro-Meso-Macroporous Zeolite CaA for Methanol Conversion to Dimethyl Ether

    Directory of Open Access Journals (Sweden)

    Yan Wang

    2016-11-01

    Full Text Available A hierarchical zeolite CaA with microporous, mesoporous and macroporous structure was hydrothermally synthesized by a ”Bond-Blocking” method using organo-functionalized mesoporous silica (MS as a silica source. The characterization by XRD, SEM/TEM and N2 adsorption/desorption techniques showed that the prepared material had well-crystalline zeolite Linde Type A (LTA topological structure, microspherical particle morphologies, and hierarchically intracrystalline micro-meso-macropores structure. With the Bond-Blocking principle, the external surface area and macro-mesoporosity of the hierarchical zeolite CaA can be adjusted by varying the organo-functionalized degree of the mesoporous silica surface. Similarly, the distribution of the micro-meso-macroporous structure in the zeolite CaA can be controlled purposely. Compared with the conventional microporous zeolite CaA, the hierarchical zeolite CaA as a catalyst in the conversion of methanol to dimethyl ether (DME, exhibited complete DME selectivity and stable catalytic activity with high methanol conversion. The catalytic performances of the hierarchical zeolite CaA results clearly from the micro-meso-macroporous structure, improving diffusion properties, favoring the access to the active surface and avoiding secondary reactions (no hydrocarbon products were detected after 3 h of reaction.

  19. Cu exchanged microporous titanium silicalite (TS-1) coated on polycrystalline mullite fibres as catalyst for the CO and NO conversion

    Energy Technology Data Exchange (ETDEWEB)

    Petrov, L.; Soria, J.; Cataluna, R. [Instituto de Catalisis y Petroleoquimica, CSIC, Campus Universitario de Cantoblanco, Madrid, (Spain); Dimitrov, L.; Spasov, L.; Dimitrov, P. [Institute of Catalysis, Bulgarian Academy of Sciences, Sofia (Bulgaria)

    1996-02-29

    A surface coated with TS-1 mullite fibre was prepared. From this material, a copper containing zeolite catalyst was produced by ion exchange, that was more active for carbon monoxide oxidation reaction than the noble metal containing supported catalysts. By combining the copper containing catalyst with rhodium and ceria, a catalyst for carbon monoxide oxidation and nitric oxide reduction reactions, superior in activity to noble metals supported catalysts were prepared

  20. 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.

  1. In-situ Micro-Spectroscopy on Coke Formation Processes in Zeolites

    NARCIS (Netherlands)

    Mores, D.

    2011-01-01

    Zeolite catalysts are used in a large variety of (petro-)chemical conversions. The acid sites in these materials are responsible for the chemical transformation, while their well-defined crystallographic architecture offers unique molecular size and shape selectivity. The finite availability of crud

  2. Shape-selective Valorization of Biomass-derived Glycolaldehyde using Tin-containing Zeolites

    DEFF Research Database (Denmark)

    Tolborg, Søren; Meier, Sebastian; Shunmugavel, Saravanamurugan

    2016-01-01

    A highly selective self-condensation of glycolaldehyde to different C4 molecules has been achieved using Lewis acidic stannosilicate catalysts in water at moderate temperatures (40–100 °C). The medium-sized zeolite pores (10-membered ring framework) in Sn-MFI facilitate the formation of tetrose...

  3. Effect of pretreatment conditions on the catalytic properties of zeolites in phenol arylalkylation with styrene

    Energy Technology Data Exchange (ETDEWEB)

    Kolesnichenko, N.V.; Romanovskii, B.V.; Kurashev, M.V.

    1980-04-01

    The effect of pretreatment conditions on the catalytic properties of zeolites in phenol arylalkylation with styrene was studied in a flow microreactor at 250/sup 0/C, 1 atm, 4:1 phenol/styrene, and 2.6 sec contact time. Samples of the zeolite-containing AShNTs-3 catalyst (a Soviet commercial grade) in the ammonia form calcined at 300/sup 0/C in flowing helium contained mainly protic acid sites and rapidly lost their catalytic activity. The same catalyst calcined in air at 500/sup 0/C contained mainly aprotic sites and its activity increased with time. Air calcination at 400/sup 0/C gave catalysts which contained similar concentrations of both protic and aprotic sites and showed stable activities and selectivities for the major products, i.e., 4- and 2-((GAMMA)-methylbenzyl)-phenol. The properties of a NH/sub 4/Y zeolite were less affected by thermal pretreatment. The commercial zeolite catalysts AShNTs-3 and Tseokar-2 (unexchanged with ammonia) were strongly promoted by steam and deactivated by carbon dioxide continuously added to the reaction zone. Both effects were reversible.

  4. Improved zeolite regeneration processes for preparing saturated branched-chain fatty acids

    Science.gov (United States)

    Ferrierite zeolite solid is an excellent catalyst for the skeletal isomerization of unsaturated linear-chain fatty acids (i.e., oleic acid) to unsaturated branched-chain fatty acids (i.e., iso-oleic acid) follow by hydrogenation to give saturated branched-chain fatty acids (i.e., isostearic acid). ...

  5. The influence of acidity on zeolite H-BEA catalyzed isobutane/n-butene alkylation

    NARCIS (Netherlands)

    Nivarthy, Gautam S.; Seshan, K.; Lercher, Johannes A.

    1998-01-01

    The influence of the concentration of acid sites for isobutane/n-butene alkylation on zeolite BEA with varying degrees of Na+ ion exchange is reported. All catalysts studied showed complete n-butene conversion over a significant time-on-stream. Isooctanes were the dominating products over H-BEA, whi

  6. Fixation of carbon dioxide into dimethyl carbonate over titanium-based zeolitic thiophene-benzimidazolate framework

    Science.gov (United States)

    A titanium-based zeolitic thiophene-benzimidazolate framework has been designed for the direct synthesis of dimethyl carbonate (DMC) from methanol and carbon dioxide. The developed catalyst activates carbon dioxide and delivers over 16% yield of DMC without the use of any dehydra...

  7. Characterization of coke deposited on nano-sized Pt-Pd/H-beta spent during long-chain paraffin hydroisomerization

    Energy Technology Data Exchange (ETDEWEB)

    Bauer, F.; Einicke, W.D.; Ficht, K.; Glaeser, R. [Leipzig Univ. (Germany). Inst. of Chemical Technology; Bertmer, M. [Leipzig Univ. (Germany). Inst. of Experimental Physics II; Kuchling, T. [Technische Univ. Bergakademie Freiberg (Germany). Inst. of Energy Process Engineering and Chemical Engineering

    2013-11-01

    The hydroisomerization of long-chain n-paraffins were studied in the temperature range 205- 230 C at p{sub H2}=50 bar using a bench scale trickle-bed continuous-flow reactor. The bimetallic catalysts consisted of mixtures of platinum and palladium supported on commercially available nano-sized zeolites Beta (n{sub Si}/n{sub Al} = 12 and 25) extruded with a binder ({gamma}-alumina). For hexadecane conversion, high yields to isomers (25 and 45 wt.% of mono- and multibranched isomers, respectively) without extensive cracking (>10 wt.%) were obtained at a conversion of 80 %. Long-term tests with C{sub 16}H{sub 34} and blends of solid n-paraffins for 30-60 days on stream clearly indicate that a minor loss in catalyst activity can easily be compensated by increasing the reaction temperature from 230 C to 235 C. The zeolite sample with a 'mild acidity' revealed low hydrocracking at isomerization yield up to 70 wt.% and high stability. Carbonaceous deposits formed during n-paraffin hydroisomerization were investigated by temperature-programmed oxidation, elemental analysis, ATR-FTIR and {sup 13}C MAS NMR spectroscopy showing the formation of low-temperature, hydrogen-rich coke. (orig.)

  8. State of the art of Lewis acid-containing zeolites: lessons from fine chemistry to new biomass transformation processes.

    Science.gov (United States)

    Moliner, Manuel

    2014-03-21

    The former synthesis of TS-1 opened new catalytic opportunities for zeolites, especially for their application as selective redox catalysts in several fine chemistry processes. Interestingly, isolated Ti species in the framework positions of hydrophobic zeolites, such as high silica zeolites, offer unique Lewis acid sites even in the presence of protic polar solvents (such as water). Following this discovery, other transition metals (such as Sn, Zr, V, Nb, among others) have been introduced in the framework positions of different hydrophobic zeolitic structures, allowing their application in new fine chemistry processes as very active and selective redox catalysts. Recently, these hydrophobic metallozeolites have been successfully applied as efficient catalysts for several biomass-transformation processes in bulk water. The acquired knowledge from the former catalytic descriptions in fine chemistry processes using hydrophobic Lewis acid-containing zeolites has been essential for their application in these novel biomass transformations. In the present review, I will describe the recent advances in the synthesis of new transition metal-containing zeolites presenting Lewis acid character, and their unique catalytic applications in both fine chemistry and novel biomass-transformations.

  9. Re/HZSM-5: a new catalyst for ethane aromatization with improved stability

    DEFF Research Database (Denmark)

    Krogh, Anne; Hansen, Thomas W.; Christensen, Claus Hviid

    2003-01-01

    Rhenium-impregnated HZSM-5 is found to be a promising catalyst for ethane aromatization. The Re–HZSM-5 catalyst deactivates significantly slower than well-known ethane aromatization Zn–HZSM-5 catalyst. Product selectivities for the two catalysts are similar, indicating that the shape selectivity...... and acid-function of the zeolite are the determining factors, and the metal function is only responsible for the activation of ethane by dehydrogenation to ethylene....

  10. Enhanced relative photonic efficiency of titania/zeolite composite photocatalysts

    Energy Technology Data Exchange (ETDEWEB)

    Shankar, M.V.; Cheralathan, K.K.; Arabindoo, B.; Palanichamy, M.; Murugesan, V. [Dept. of Chemistry, Anna Univ., Chennai (India)

    2003-07-01

    The photocatalytic degradation of 2,4-dichlorophenoxyacetic acid, an endocrine disrupter using TiO{sub 2} and supported TiO{sub 2} has been attempted in the present investigation. Batch studies were carried out to optimise various experimental parameters for maximum degradation efficiency. As the adsorption capacity of the photocatalyst is important to provide maximum pollutant concentration environment surrounding the catalyst, zeolites, which are good adsorbents were chosen as supports for TiO{sub 2}. Studies were conducted with three different zeolites differing in Si/Al ratio which governs the hydrophilicity of the support. The wt% loading of TiO{sub 2} on the support was found to be important for effective degradation. Though immobilised system requires high wt% loading the amount of TiO{sub 2} used is only 50% compared to TiO{sub 2} system. Zeolite being less expensive than TiO{sub 2}, TiO{sub 2}/zeolite composite system makes the process cost effective. The efficiencies of various systems were compared in terms of relative photonic efficiency. The relative photonic efficiency value for all these systems is more than one showing the effectiveness of this process. (orig.)

  11. Catalytic pyrolysis using UZM-44 aluminosilicate zeolite

    Science.gov (United States)

    Nicholas, Christopher P; Boldingh, Edwin P

    2013-12-17

    A new family of aluminosilicate zeolites designated UZM-44 has been synthesized. These zeolites are represented by the empirical formula Na.sub.nM.sub.m.sup.k+T.sub.tAl.sub.1-xE.sub.xSi.sub.yO.sub.z where "n" is the mole ratio of Na to (Al+E), M represents a metal or metals from zinc, Group 1, Group 2, Group 3 and or the lanthanide series of the periodic table, "m" is the mole ratio of M to (Al+E), "k" is the average charge of the metal or metals M, T is the organic structure directing agent or agents, and E is a framework element such as gallium. The process involves contacting a carbonaceous biomass feedstock with UZM-44 at pyrolysis conditions to produce pyrolysis gases comprising hydrocarbons. The catalyst catalyzes a deoxygenation reaction converting oxygenated hydrocarbons into hydrocarbons and removing the oxygen as carbon oxides and water. A portion of the pyrolysis gases is condensed to produce low oxygen biomass-derived pyrolysis oil.

  12. Catalytic pyrolysis using UZM-44 aluminosilicate zeolite

    Energy Technology Data Exchange (ETDEWEB)

    Nicholas, Christopher P; Boldingh, Edwin P

    2014-04-29

    A new family of aluminosilicate zeolites designated UZM-44 has been synthesized. These zeolites are represented by the empirical formula. Na.sub.nM.sub.m.sup.k+T.sub.tAl.sub.1-xE.sub.xSi.sub.yO.sub.z where "n" is the mole ratio of Na to (Al+E), M represents a metal or metals from zinc, Group 1, Group 2, Group 3 and or the lanthanide series of the periodic table, "m" is the mole ratio of M to (Al+E), "k" is the average charge of the metal or metals M, T is the organic structure directing agent or agents, and E is a framework element such as gallium. The process involves contacting a carbonaceous biomass feedstock with UZM-44 at pyrolysis conditions to produce pyrolysis gases comprising hydrocarbons. The catalyst catalyzes a deoxygenation reaction converting oxygenated hydrocarbons into hydrocarbons and removing the oxygen as carbon oxides and water. A portion of the pyrolysis gases is condensed to produce low oxygen biomass-derived pyrolysis oil.

  13. Platinum incorporation in the Na Y zeolite through impregnation method, and characterization by XRD, FTIR and nitrogen adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Araujo, A.S.; Sousa, B.V.; Andrade, A.C.C.; Rodrigues, M.G.F. [Universidade Federal de Campina Grande (UFCG), PB (Brazil). Centro de Ciencias e Tecnologia. Unidade Academica de Engenharia Quimica], e-mail: alfredinad@yahoo.com.br, e-mail: biancaviana_cg@yahoo.com.br, e-mail: meiry@deq.ufcg.edu.br; Rangel, M.C. [Universidade Federal da Bahia (UFBA), Salvador, BA (Brazil). Inst. de Quimica. Grupo de Estudos em Cinetica e Catalise

    2007-07-01

    Supported metal catalysts are widely used in petroleum refining, chemical and petroleum industries. These catalysts are important in ammonia synthesis, conversion of hydrocarbons with water vapor to synthesis gas, reforming, hydrocracking, ... Platinum has long been used in cracking, hydrogenation and dehydrogenation processes. The aim of this project is the Na Y zeolitic sample preparation through impregnation for incipient humidity, with 0,5% concentration of platinum, aiming its use as a catalyst in the steam reforming reaction. The characterization techniques used were: X Rays Diffraction (XRD), Fourier Transform Infrared spectroscopy (FTIR) and Nitrogen Adsorption (BET Method). From the obtained results through the techniques mentioned previously it is possible to evidence that the platinum impregnation process did not change the Na Y zeolite structure. Through the superficial specific area (BET) it was possible to observe that the platinum impregnation process caused a decrease in the specific area due to the reduction to the accessibility to the micropores of the zeolitic structure. (author)

  14. Determination of the maximum retention of cobalt by ion exchange in h-zeolites

    Directory of Open Access Journals (Sweden)

    A. S. Zola

    2012-06-01

    Full Text Available This work aimed to determine the maximum content of cobalt that can be incorporated by ion exchange in zeolites H-USY, H-Beta, H-Mordenite, and H-ZSM-5. To reach this goal, batch isotherms at 75ºC were constructed after addition of zeolite samples in flasks filled with cobalt nitrate solution. The equilibrium data were fitted to Langmuir, Freundlich, and Tóth adsorption isotherm models. Langmuir was the best model for zeolites H-Beta, H-Mordenite, and H-ZSM-5, whereas experimental data for H-USY were better fitted to the Freundlich isotherm model. From the isotherms, it was possible to determine the maximum cobalt exchange level (q max that can be incorporated in each zeolite through ion exchange. In this sense, H-USY presented the highest q max value (2.40 meq/g zeol, while H-ZSM-5 showed the lowest one (0.64 meq/g zeol. These results also show the influence of the zeolite framework related to the channel system, pore opening, presence of cavities and secondary porosity and SiO2/Al2O3 ratio (SAR on the maximum capacity and behavior of cobalt ion exchange in protonic zeolites.

  15. Granulated zeolite plant "Alusil", Zvornik

    Directory of Open Access Journals (Sweden)

    Stanković Mirjana S.

    2003-01-01

    Full Text Available The IGPC's Engineering Department designed basic technological and machine projects for a granulated zeolite production plant, on the basis of which a pilot plant with an initial capacity of 5,000 t/y was constructed in 1984, within Birač - Zvornik production complex. The technology in these projects was developed in the laboratories of the IGPC.Several goals were realized by designing a granulated zeolite production plant. This technology is one of the newest state of the art high tech technologies. The product meets all quality demands, as well as environmental regulations, by which granulated zeolite production for various uses was developed. The granulated zeolite production process is fully automatized, and the product has uniform quality. There is no waste material in granulated zeolite production, because all products with unsatisfactory quality are returned to the process. The production process can be controlled manually, which is necessary during start - up, and repairs.

  16. Method for producing zeolites and zeotypes

    DEFF Research Database (Denmark)

    2015-01-01

    The invention relates to a method for producing zeolite, zeolite-like or zeotype particles comprising the steps of: 1 ) Adding one or more metal precursors to a silica or alumina source; 2) Reducing the one or more metal precursors to form metal nanoparticles on the surface of the silica or alumina...... source; 3) Passing a gaseous hydrocarbon, alkyl alcohol or alkyl ether over the silica or alumina supported metal nanoparticle to form a carbon template coated zeolite, zeolite-like or zeotype precursor composition; 4a) Adding a structure directing agent to the carbon template coated zeolite, zeolite......-like or zeotype precursor composition thereby creating a zeolite, zeolite-like or zeotype gel composition; 4b) Crystallising the zeolite, zeolite-like or zeotype gel composition by subjecting said composition to a hydrothermal treatment; 5) Removing the carbon template and structure directing agent and isolating...

  17. Time- and space-resolved study of the methanol to hydrocarbons (MTH) reaction - influence of zeolite topology on axial deactivation patterns.

    Science.gov (United States)

    Rojo-Gama, Daniel; Etemadi, Samaneh; Kirby, Eliot; Lillerud, Karl Petter; Beato, Pablo; Svelle, Stian; Olsbye, Unni

    2017-02-10

    Zeolites representing seven different topologies were subjected to life-time assessment studies as methanol to hydrocarbons (MTH) catalysts at 400 °C, P(MeOH) = 13 kPa and P(tot) = 100 kPa. The following topologies were studied: ZSM-22 (TON), ZSM-23 (MTT), IM-5 (IMF), ITQ-13 (ITH), ZSM-5 (MFI), mordenite (MOR) and beta (BEA). Two experimental approaches were used. In the first approach, each catalyst was tested at three different contact times, all giving 100% initial conversion. The life-time before conversion decreased to 50% at each contact time was measured and used to calculate critical contact times (i.e. the contact time needed to launch the autocatalytic MTH reaction) and deactivation rates. It was found that the critical contact time is strongly correlated with pore size: the smaller the pore size, the longer the critical contact time. The second experimental approach consisted of testing the catalysts in a double tube reactor with 100% initial conversion, and quenching the reaction after 4 consecutive times on stream, representing full, partial, and zero conversion. After quenching, the catalyst bed was divided into four segments, which were individually characterised for coke content (temperature-programmed oxidation) and specific surface area (N2 adsorption). The axial deactivation pattern was found to depend on pore size. With increasing pore size, the main source of coke formation changed from methanol conversion (1D 10-ring structures), to partly methanol, partly product conversion (3D 10-ring structures) and finally mainly product conversion (3D 12-ring structure). As a result, the methanol conversion capacity changed little with contact time for ZSM-5, while it increased with increasing contact time for the catalysts with smaller pore sizes, and decreased with increasing contact time for pore sizes larger than ZSM-5.

  18. Understanding the dissolution of zeolites.

    Science.gov (United States)

    Hartman, Ryan L; Fogler, H Scott

    2007-05-08

    Scientific knowledge of how zeolites, a unique classification of microporous aluminosilicates, undergo dissolution in aqueous hydrochloric acid solutions is limited. Understanding the dissolution of zeolites is fundamental to a number of processes occurring in nature and throughout industry. To better understand the dissolution process, experiments were carried out establishing that the Si-to-Al ratio controls zeolite framework dissolution, by which the selective removal of aluminum constrains the removal of silicon. Stoichiometric dissolution is observed for Type 4A zeolite in HCl where the Si-to-Al ratio is equal to 1.0. Framework silicon dissolves completely during Type 4A dissolution and is followed by silicate precipitation. However, for the zeolite analcime which has a Si-to-Al ratio of 2.0 dissolves non-stoichiometrically as the selective removal of aluminum results in partially dissolved silicate particles followed by silicate precipitation. In Type Y zeolite, exhibiting a Si-to-Al ratio of 3.0, there is insufficient aluminum to weaken the structure and cause silicon to dissolve in HCl. Thus, little or no precipitation is observed, and amorphous undissolvable silicate particles remain intact. The initial dissolution rates of Type Y and 4A zeolites demonstrate that dissolution is constrained by the number of available reaction sites, and a selective removal rate parameter is applied to delineate the mechanism of particle dissolution by demonstrating the kinetic influence of the Si-to-Al ratio. Zeolite framework models are constructed and used to undergird the basic dissolution mechanism. The framework models, scanning electron micrographs of partially dissolved crystals, and experimentally measured dissolution rates all demonstrate that a zeolite's Si-to-Al framework ratio plays a universal role in the dissolution mechanism, independent of framework type. Consequently, the unique mechanism of zeolite dissolution has general implications on how petroleum

  19. Oxygen and hydrogen isotope geochemistry of zeolites

    Science.gov (United States)

    Karlsson, Haraldur R.; Clayton, Robert N.

    1990-01-01

    Oxygen and hydrogen isotope ratios for natural samples of the zeolites analcime, chabazite, clinoptilolite, laumontite, mordenite, and natrolite have been obtained. The zeolite samples were classified into sedimentary, hydrothermal, and igneous groups. The ratios for each species of zeolite are reported. The results are used to discuss the origin of channel water, the role of zeolites in water-rock interaction, and the possibility that a calibrated zeolite could be used as a low-temperature geothermometer.

  20. Lewis-acid and redox-active zeolite catalysts for the activation of methane and lower hydrocarbons in the selective catalytic reduction of NO{sub x}. Subproject: structural characterization and kinetic modelling. Final report; Lewis-acide und redox-aktive Zeolith-Katalysatoren fuer die Aktivierung von Methan und Fluessiggas-Kohlenwasserstoffen in der SCR von NO{sub x}. Teilprojekt: Strukturelle Katalysatorcharakterisierung und Modellierung der Reaktionskinetik. Abschlussbericht

    Energy Technology Data Exchange (ETDEWEB)

    Gruenert, W. [Bochum Univ. (Germany). Technische Chemie; Sowade, T.; Schmidt, C.; Stroeder, U. [Heraeus (W.C.) GmbH, Hanau (Germany)

    2001-12-01

    Zeolites (in particular ZSM-5) modified by indium and additionally promoted by ceria have been studied as catalysts for selective reduction of NO by methane. The structural properties of the catalysts have been investigated by XRD, FTIR, EXAFS, electron microscopy and XPS. The ceria promotor may be added to In-ZSM-5 by precipitation onto the external zeolite surface or by physically admixing a high surface-area powder. The preparation of the basic In-ZSM-5 system has a large influence on the properties of the catalyst. Preparation by aqueous exchange leads in most cases to a coexistence of a small amount of intra-zeolite indium species and extra-zeolite indium phases. Only at low pH, exclusively intra-zeolite indium is formed to a low extent (<10% exchange degree). Intrazeolite indium can be also obtained by dry preparations using InCl{sub 3} (solid-state ion exchange, sublimation, transport reaction). The In species formed carry Cl ligands, the stability of which depends on the indium content: after washing and calcination steps, Cl ligands could no longer be detected only in samples with low In content. Reductive solid-state ion exchange is a further method to prepare intra-zeolite In species. In mixtures containing excess indium, oligometric intra-zeolite In species are formed via this route. Intra-zeolite Cl-free In species exhibit significant SCR activity while Cl-containing In-species activate methane with low SCR selectivity. In ceria-promoted systems, the ceria provides full NO{sub 2} supply by catalysing the NO oxidation. With sufficient NO{sub 2} supply, the even Cl-containing In sites provide high SCR activities. Since the relevance of acidic sites was established e.g. by poisoning experiments, the reaction mechanism can by visualised by proceeding via methane activation over In sites, reaction of activated methane with NO{sub 2} to a volatile intermediate (e.g. nitromethane), which is then decomposed over the acidic sites. The reaction kinetics of the

  1. MMC-High Propylene Selectivity DCC Catalyst

    Institute of Scientific and Technical Information of China (English)

    Li Zheng; Xie Chaogang; Luo Yibin; Zhao Liuzhou; Shu Xingtian

    2007-01-01

    RIPP has developed the third generation novel DCC catalysts aimed at increasing the propylene yield, named as the MMC series catalysts. This catalyst is of the MFI structure composed of the ZSP zeolite as the main active component, which has higher capability for producing low-carbon olefins, in particular the propylene. The commercial application of this catalyst at SINOPEC Anqing Petrochemical Company has revealed that the adoption of the MMC-2 catalyst has resulted in a 1.6-4.0 percentages increase in propylene yield under basically similar conditions in terms of the feedstock property and process operating regime coupled with reduction in gasoline olefin content and increase in aromatic content to improve the gasoline quality.

  2. Shape-selective zeolite catalysis for bioplastics production

    Science.gov (United States)

    Dusselier, Michiel; Van Wouwe, Pieter; Dewaele, Annelies; Jacobs, Pierre A.; Sels, Bert F.

    2015-07-01

    Biodegradable and renewable polymers, such as polylactic acid, are benign alternatives for petrochemical-based plastics. Current production of polylactic acid via its key building block lactide, the cyclic dimer of lactic acid, is inefficient in terms of energy, time, and feedstock use. We present a direct zeolite-based catalytic process, which converts lactic acid into lactide. The shape-selective properties of zeolites are essential to attain record lactide yields, outperforming those of the current multistep process by avoiding both racemization and side-product formation. The highly productive process is strengthened by facile recovery and practical reactivation of the catalyst, which remains structurally fit during at least six consecutive reactions, and by the ease of solvent and side-product recycling.

  3. Hierarchical zeolites and their catalytic performance in selective oxidative processes.

    Science.gov (United States)

    Ojeda, Manuel; Grau-Atienza, Aida; Campos, Rafael; Romero, Antonio A; Serrano, Elena; Maria Marinas, Jose; García Martínez, Javier; Luque, Rafael

    2015-04-24

    Hierarchical ZSM-5 zeolites prepared using a simple alkali treatment and subsequent HCl washing are found to exhibit unprecedented catalytic activities in selective oxidation of benzyl alcohol under microwave irradiation. The metal-free zeolites promote the microwave-assisted oxidation of benzyl alcohol with hydrogen peroxide in yields ranging from 45-35 % after 5 min of reaction under mild reaction conditions as well as the epoxidation of cyclohexene to valuable products (40-60 % conversion). The hierarchically porous systems also exhibited an interesting catalytic activity in the dehydration of N,N-dimethylformamide (25-30 % conversion), representing the first example of transition-metal free catalysts in this reaction.

  4. Zeolite-Catalyzed Hydrocarbon Formation from Methanol: Density Functional Simulations

    Directory of Open Access Journals (Sweden)

    George Fitzgerald

    2002-04-01

    Full Text Available Abstract: We report detailed density functional theory (DFT calculations of important mechanisms in the methanol to gasoline (MTG process in a zeolite catalyst. Various reaction paths and energy barriers involving C-O bond cleavage and the first C-C bond formation are investigated in detail using all-electron periodic supercell calculations and recently developed geometry optimization and transition state search algorithms. We have further investigated the formation of ethanol and have identified a different mechanism than previously reported [1], a reaction where water does not play any visible role. Contrary to recent cluster calculations, we were not able to find a stable surface ylide structure. However, a stable ylide structure built into the zeolite framework was found to be possible, albeit a very high reaction barrier.

  5. GREEN CHEMISTRY. Shape-selective zeolite catalysis for bioplastics production.

    Science.gov (United States)

    Dusselier, Michiel; Van Wouwe, Pieter; Dewaele, Annelies; Jacobs, Pierre A; Sels, Bert F

    2015-07-03

    Biodegradable and renewable polymers, such as polylactic acid, are benign alternatives for petrochemical-based plastics. Current production of polylactic acid via its key building block lactide, the cyclic dimer of lactic acid, is inefficient in terms of energy, time, and feedstock use. We present a direct zeolite-based catalytic process, which converts lactic acid into lactide. The shape-selective properties of zeolites are essential to attain record lactide yields, outperforming those of the current multistep process by avoiding both racemization and side-product formation. The highly productive process is strengthened by facile recovery and practical reactivation of the catalyst, which remains structurally fit during at least six consecutive reactions, and by the ease of solvent and side-product recycling.

  6. Isobutane/2-butene alkylation in Y zeolite exchange with metallic ions; Alquilacao de isobutano com 2-buteno em zeolita Y trocada com ions metalicos

    Energy Technology Data Exchange (ETDEWEB)

    Rosenbach Junior, Nilton; Mota, Claudio J.A. [Universidade Federal, Rio de Janeiro, RJ (Brazil). Inst. de Quimica]. E-mail: cmota@iq.ufrj.br

    2003-07-01

    In industrial scale-process, isobutane/2-butene alkylation has been normally achieved under strong acids conditions, using HF or H{sub 2}SO{sub 4} as catalysts. Nevertheless, this acids present problems such as high consumption and environmental risk. Therefore, there is a strong interest in substituting them by solid catalysts. However, over solid acids, there is a fast deactivation, usually attributed to oligomerization, occurring on Broensted sites, that preferentially adsorb the unsaturated hydrocarbons. This study shows that the reaction can occur on zeolites Y without Broensted acid sites, using an alkyl halide as initiator, added to the feed in the initial moments of the reaction. In this approach the oligomerization problem is minimized. The reactions were carried out in liquid phase at 50 deg C and 450 lb/in{sup 2}, using a mixture of isobutene/2-butene with a molar fraction of 10:1. Catalyst activity and selectivity to trimethylpentane and dimethylhexane for the Y zeolite exchange with Ag{sup +}, Cu{sup ++} and Fe{sup +++} were followed by on line capillary gas chromatography. For comparison purpose, the reaction was also carried out on a HUSY zeolite. All cation-exchanged zeolite presented a better performance than the protonic zeolite. The best performance was of the Y zeolite exchange with Ag{sup +}, followed by Cu{sup ++} and Fe{sup +++} exchanged zeolites. (author)

  7. Decoupling HZSM-5 catalyst activity from deactivation during upgrading of pyrolysis oil vapors.

    Science.gov (United States)

    Wan, Shaolong; Waters, Christopher; Stevens, Adam; Gumidyala, Abhishek; Jentoft, Rolf; Lobban, Lance; Resasco, Daniel; Mallinson, Richard; Crossley, Steven

    2015-02-01

    The independent evaluation of catalyst activity and stability during the catalytic pyrolysis of biomass is challenging because of the nature of the reaction system and rapid catalyst deactivation that force the use of excess catalyst. In this contribution we use a modified pyroprobe system in which pulses of pyrolysis vapors are converted over a series of HZSM-5 catalysts in a separate fixed-bed reactor controlled independently. Both the reactor-bed temperature and the Si/Al ratio of the zeolite are varied to evaluate catalyst activity and deactivation rates independently both on a constant surface area and constant acid site basis. Results show that there is an optimum catalyst-bed temperature for the production of aromatics, above which the production of light gases increases and that of aromatics decrease. Zeolites with lower Si/Al ratios give comparable initial rates for aromatics production, but far more rapid catalyst deactivation rates than those with higher Si/Al ratios.

  8. Regeneration of Hydrotreating and FCC Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    CM Wai; JG Frye; JL Fulton; LE Bowman; LJ Silva; MA Gerber

    1999-09-30

    -earth exchanged Y zeolite in a silica-alumina matrix. X-ray fluorescence analyses showed that the rare earths used in preparing the catalysts were a mixture of lanthanum and cerium. Antimony found in the spent catalyst was added during operation of the FCC unit as a way to suppress the adverse effects of deposited nickel. The fresh HDS samples consisted of sulfided nickel and molybdenum on an alumina support. The spent catalyst showed nearly 10% vanadium on the catalyst and a modest increase in nickel and sulfur on the catalyst as a result of operations. Hydrocracking catalysts were not available for this study.

  9. Methyl Halide to Olefins and Gasoline over Zeolites and SAPO Catalysts: A New Route of MTO and MTG%沸石和SAPO分子筛催化卤代甲烷转化制烯烃和汽油:一种新的MTO和MTG路线

    Institute of Scientific and Technical Information of China (English)

    魏迎旭; 张大治; 刘中民; 苏宝连

    2012-01-01

    Rational and efficient conversion of methane to more useful higher hydrocarbons is one of the most important topics of natural gas utilization.Although methane activation and its conversion to valuable compounds attract an increasing attention,methane conversion is often made in indirect way through the very energy-consuming step for syngas production from steam reforming of methane.Some promising results appeared to be of significance for the development of an alternative and potential route for the production of high value-added products from methane.Efficient conversion of methane to higher hydrocarbons could be realized via methyl halide as the intermediate.After the production of halomethane,they could be transformed to gasoline and light olefins over modified zeolites and SAPO molecular sieves.High conversion efficiency and selectivity indicated the feasibility of industrial application.The research gained recently growing interest from the point of view in both fundamental research and industrial application.The study on the reaction mechanism shed light on the possible route of C-C bond construction from methyl halide,which is the very important issue of the C1-reactant conversion to higher hydrocarbons.Hydrogen halide generation during methyl halide conversion did not exert apparent impact on the reaction mechanism and the structure stability of the catalysts.This review deals with the evolution of the field and comments the advantages to be explored and the drawbacks to be prevented for the development of new and sustainable methane-to-olefins (MTO) and methane-to-gasoline (MTG) routes via methyl halides.

  10. The potential of medium-pore zeolites for improved propene yields from catalytic cracking

    Energy Technology Data Exchange (ETDEWEB)

    Bager, F.; Salas, N.; Ernst, S. [Technische Univ. Kaiserslautern (Germany). Dept. of Chemistry, Chemical Technology

    2011-07-01

    The medium-pore zeolites ZSM-5 (MFI), ZSM-22 (TON), ZSM-23 (MTT), and EU-1 (EUO) were synthesized under hydrothermal conditions and modified by ion exchange to obtain the Broensted-acid forms. The activity and selectivity of these catalysts in catalytic cracking of a model compound, viz. n-octane, was studied in a fixed-bed flow-type reactor. The catalytic results clearly reflect the differences in the pore architectures of the tested zeolites on n-octane conversion and on the product selectivities. Over the zeolites with one-dimensional pore systems and without large intracrystalline cavities, a remarkable increase of the contribution of the monomolecular cracking mechanism could be observed as compared to the standard catalyst zeolite ZSM-5. This is indicated by a high selectivity for unsaturated products and, hence, increasing yields of propene. Large cavities in the pore system, viz. in the case of zeolite EU-1, increase the conversion in particular at lower temperatures. However, the large cavities also favor the formation of large transition states required for the classical bimolecular cracking mechanism, resulting in decreased selectivities for unsaturated products, increased selectivities for aromatics formation and faster deactivation. (orig.)

  11. KINETIKA REAKSI PADA PROSES PRODUKSI DIETIL ETER DARI ETANOL DENGAN KATALIS H-ZEOLIT

    Directory of Open Access Journals (Sweden)

    Widayat Widayat

    2012-11-01

    Full Text Available DiEtil Eter diproduksi dari etanol dengan proses dehidrasi. Penelitian ini bertujuan untukmempelajari kinetika reaksi proses dehidrasi etanol dengan katalis H-zeolit. Katalis H-zeolitdisintesis dengan proses dealuminasi dan kalsinasi dan impregnasi dengan logam Al dan prosesreduksi dan kalsinasi. Proses produksi DiEtil Eter dilaksanakan dengan proses adsorpsi dan reaksikatalitik sedangkan proses studi kinetika reaksi menggunakan pendekatan Langmuir-Hinshelwood.Proses analisis kinetika reaksi menggunakan perangkat lunak MATLAB. Model kinetika reaksi prosesdehidrasi etanol menjadi DiEtil Eter dan etilen dengan katalis H-zeolit pada konsentrasi umpanetanol 85-95% dan rentang temperatur 140-240oC, dimana reaksi permukaan yang mengontrol reaksiglobal adalahDiEthyl Ether is produced by using ethanol dehydrationprocess. The objective of this research was to study the reaction kinetic of ethanol dehydrationprocess by H-zeolite catalyst from natural zeolite. The H-zeolite catalyst was prepared bydealumination, calcination, impregnation with Al and reduction processes. DiEthyl Ether productionwas produced by using adsorption-catalytic reaction. The kinetic study was did with MATLABsoftware. Kinetic model of ethanol dehydration processes into DiEthyl Ether and ethylene with Hzeolitecatalyst and ethanol feed concentration among 85-95% and temperature between 140-240oCunder surface reaction is shown by

  12. Alternative alkali resistant deNOx catalysts

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Kristensen, Steffen Buus; Due-Hansen, Johannes;

    2012-01-01

    Alternative alkali resistant deNOx catalysts were prepared using three different supports ZrO2, TiO2 and Mordenite zeolite. The majority of the catalysts were prepared by incipient wetness impregnation of a commercial support, with vanadium, copper or iron precursor, one catalyst was prepared...... by onepot sol–gel method. All catalysts were characterized by BET, XRPD and NH3-TPD. Initial SCR activities of 8 out of 9 catalysts showed higher NO conversion at least at one temperature in the temperature range 300–500 ◦C compared to the conventional V2O5-WO3/TiO2 catalyst. After potassium poisoning (100......–130 µmol of K/g of catalyst) the relative drop in SCR activity and acidity was lower for all the alternative catalysts compared to the industrial V2O5-WO3/TiO2 catalyst. Furthermore, Cu/MOR and Nano-V2O5/Sul-TiO2 catalysts showed 8–16 times higher SCR activities than the conventional even after high...

  13. Properties and applications of zeolites.

    Science.gov (United States)

    Rhodes, Christopher J

    2010-01-01

    Zeolites are aluminosilicate solids bearing a negatively charged honeycomb framework of micropores into which molecules may be adsorbed for environmental decontamination, and to catalyse chemical reactions. They are central to green-chemistry since the necessity for organic solvents is minimised. Proton-exchanged (H) zeolites are extensively employed in the petrochemical industry for cracking crude oil fractions into fuels and chemical feedstocks for other industrial processes. Due to their ability to perform cation-exchange, in which the cations that are originally present to counterbalance the framework negative charge may be exchanged out of the zeolite by cations present in aqueous solution, zeolites are useful as industrial water-softeners, in the removal of radioactive Cs+ and Sr2+ cations from liquid nuclear waste and in the removal of toxic heavy metal cations from groundwaters and run-off waters. Surfactant-modified zeolites (SMZ) find particular application in the co-removal of both toxic anions and organic pollutants. Toxic anions such as arsenite, arsenate, chromate, cyanide and radioactive iodide can also be removed by adsorption into zeolites that have been previously loaded with co-precipitating metal cations such as Ag+ and Pb2+ which form practically insoluble complexes that are contained within the zeolite matrix.

  14. Functionalized Cellulose: PET Polymer Fibers with Zeolites for Detoxification Against Nerve Agents%Functionalized Cellulose:PET Polymer Fibers with Zeolites for Detoxification Against Nerve Agents

    Institute of Scientific and Technical Information of China (English)

    Agarwal Satya R; Sundarrajan Subramanian; Ramakrishna Seeram

    2012-01-01

    Presently activated carbon is used as an adsorptive material for chemical and biological warfare agents.It possess excellent surface properties such as large surface area,fire-resistance and plenty availability,but has disadvantages such as its heavy weight,low breathability (after adsorption of moisture) and disposal.In this paper,we propose to utilize novel electrospun polymeric nanostructures having zeolites as catalyst materials.In this respective,the electrospun polymer nanofibers would serve as the best possible substitutes to activated carbon based protective clothing applications.This is the first in the literature that reports the integration of these types of catalysts with nanofiberous membranes.Electrospinning of cellulose/polyethylene terephthalate (PET) blend nanofibers has been carried out.Zeolite catalysts (Linde Type A and Mordenite) for the detoxification of nerve agent stimulant-paraoxon,were prepared due to their relative simplicity of synthesis.The catalysts were then coated onto nanofiber membranes and their morphology was confirmed using SEM.This is the first report on the coating of nanofibers with zeolites and their successful demonstration against nerve agent stimulant.The UV absorption spectra clearly show the detoxification ability of the functionalized fibers and their potential to be used in textiles for protection and decontamination.

  15. Oxygen-containing coke species in zeolite-catalyzed conversion of methanol to hydrocarbons

    KAUST Repository

    Liu, Zhaohui

    2016-10-06

    Zeolites are the most commonly used catalysts for methanol-to-hydrocarbon (MTH) conversion. Here, we identified two oxygen-containing compounds as coke species in zeolite catalysts after MTH reactions. We investigated the possible influences of the oxygen-containing compounds on coke formation, catalyst deactivation, product selectivity, and the induction period of the MTH reaction through a series of controlled experiments in which one of the identified compounds (2,3-dimethyl-2-cyclopenten-1-one) was co-fed with methanol over a zeolite H-ZSM-5 catalyst. Our results allow us to infer that once produced, the oxygen-containing compounds block the Brønsted acid sites by strong chemisorption and their rapid conversion to aromatics expedites the formation of coke and thus the deactivation of the catalyst. A minor effect of the production of such compounds during the MTH reaction is that the aromatic-based catalytic cycle can be slightly promoted to give higher selectivity to ethylene.

  16. Oxidation of benzyl alcohol by K2FeO4 to benzaldehyde over zeolites

    Science.gov (United States)

    Wang, Yuan-Yuan; Song, Hua; Song, Hua-Lin; Jin, Zai-Shun

    2016-10-01

    A novel and green procedure for benzaldehyde synthesis by potassium ferrate oxidation of benzyl alcohol employing zeolite catalysts was studied. The prepared oxidant was characterized by SEM and XRD. The catalytic activity of various solid catalysts was studied using benzyl alcohol as a model compound. USY was found to be a very efficient catalyst for this particular oxidation process. Benzaldehyde yields up to 96.0% could be obtained at the following optimal conditions: 0.2 mL of benzyl alcohol, 4 mmol of K2FeO4, 0.5 g of USY zeolite; 20 mL of cyclohexene, 0.3 mL of acetic acid (36 wt %), 30°C temperature, 4 h reaction time.

  17. OPTIMASI TEMPERATUR HIDRODESULFURISASI TIOFEN TERKATALISIS NI-MO/ZEOLIT ALAM

    Directory of Open Access Journals (Sweden)

    Harjito -

    2013-07-01

    Full Text Available Telah dilakukan kajian mengenai pengaruh temperatur hidrodesulfurisasi terhadap produk hidrodesulfurisasi tiofen. Penelitian dilakukan untuk mengetahui temperatur optimum hidrodesulfurisasi tiofen dengan katalis Ni-Mo/zeolite alam. Variasi temperatur yang dilakukan adalah 3000C, 3500Cdan 4000C. Katalis Ni-Mo/Zeolit alam dipreparasi secara koimpregnasi. Proses hidrodesulfurisasi dilakukan dengan umpan campuran tiofen-n-heksan dengan komposisi 1:1. Sebagai gas pembawa digunakan gas hydrogen dengan laju alir 25 mL/menit. Hasil hidrodesulfurisasi didinginkan dan dianalisis dengan kromatografi gas. Hasil analisis menunjukkan terjadinya peningkatan jumlah produk dan komponen produk pada setiap kenaikan temperatur 500C. Namun demikian kenaikan jumlah produk pada kenaikan temperatur dari 3500C ke 4000C jika dibandingkan dengan kenaikan produk pada kenaikan temperatur dari 3000C ke 3500C tidak cukup signifikan. Jadi dapat disimpulkan bahwa temperatur hidrodesulfurisasi tiofen terkatalisis Ni-Mo/Zeolit alam adalah 3500C. The study on the effect of temperature on the product tiofen hydrodesulfurization by using Ni/Mo/natural tiofen-n-hexane. The study was done conducted to determine the optimum temperature of  hydrodesulfurization tiofen by using Ni-Mo/ natural zeolite catalyst and the temperature variation was 300oC, 350oC dan 400oC. The Ni-Mo/ natural Zeolit  catalysts were prepared by coimpregnation and hydrodesulfurization process was done by tiofen-n-hexane feed mixture with composition of 1:1, hydrogen gas was used as a carrier gas with a flow rate 25 ml/min. The result of  hydrodesulfurization was cooled and analyzed by gas chromatography  and it revealed an increasing number of products and product components at for each 50°C rising of temperature. However, the increasing of number of products on the temperature rise of  350°C to 400°C was not significant if compared to the increasing of product temperature that increased

  18. Phosphorus promotion and poisoning in zeolite-based materials: synthesis, characterisation and catalysis.

    Science.gov (United States)

    van der Bij, Hendrik E; Weckhuysen, Bert M

    2015-10-21

    Phosphorus and microporous aluminosilicates, better known as zeolites, have a unique but poorly understood relationship. For example, phosphatation of the industrially important zeolite H-ZSM-5 is a well-known, relatively inexpensive and seemingly straightforward post-synthetic modification applied by the chemical industry not only to alter its hydrothermal stability and acidity, but also to increase its selectivity towards light olefins in hydrocarbon catalysis. On the other hand, phosphorus poisoning of zeolite-based catalysts, which are used for removing nitrogen oxides from exhaust fuels, poses a problem for their use in diesel engine catalysts. Despite the wide impact of phosphorus-zeolite chemistry, the exact physicochemical processes that take place require a more profound understanding. This review article provides the reader with a comprehensive and state-of-the-art overview of the academic literature, from the first reports in the late 1970s until the most recent studies. In the first part an in-depth analysis is undertaken, which will reveal universal physicochemical and structural effects of phosphorus-zeolite chemistry on the framework structure, accessibility, and strength of acid sites. The second part discusses the hydrothermal stability of zeolites and clarifies the promotional role that phosphorus plays. The third part of the review paper links the structural and physicochemical effects of phosphorus on zeolite materials with their catalytic performance in a variety of catalytic processes, including alkylation of aromatics, catalytic cracking, methanol-to-hydrocarbon processing, dehydration of bioalcohol, and ammonia selective catalytic reduction (SCR) of NOx. Based on these insights, we discuss potential applications and important directions for further research.

  19. Development of GREET Catalyst Module

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Zhichao [Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division; Dunn, Jennifer B. [Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division; Cronauer, Donald C. [Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division

    2014-09-01

    Catalysts are critical inputs for many pathways that convert biomass into biofuels. Energy consumption and greenhouse gas (GHG) emissions during the production of catalysts and chemical inputs influence the life-cycle energy consumption, and GHG emissions of biofuels and need to be considered in biofuel life-cycle analysis (LCA). In this report, we develop energy and material flows for the production of three different catalysts (tar reforming, alcohol synthesis, Zeolite Socony Mobil-5 [ZSM-5]) and two chemicals (olivine, dimethyl ether of polyethylene glycol [DEPG]). These compounds and catalysts are now included in the Greenhouse Gases, Regulated Emissions and Energy Use in Transportation (GREET™) catalyst module. They were selected because they are consumed in existing U.S. Department of Energy (DOE) analyses of biofuel processes. For example, a thermochemical ethanol production pathway (indirect gasification and mixed alcohol synthesis) developed by the National Renewable Energy Laboratory (NREL) uses olivine, DEPG, and tar reforming and alcohol synthesis catalysts (Dutta et al., 2011). ZSM-5 can be used in biofuel production pathways such as catalytic upgrading of sugars into hydrocarbons (Biddy and Jones, 2013). Other uses for these compounds and catalysts are certainly possible. In this report, we document the data sources and methodology we used to develop material and energy flows for the catalysts and compounds in the GREET catalyst module. In Section 2 we focus on compounds used in the model Dutta et al. (2011) developed. In Section 3, we report material and energy flows associated with ZSM-5 production. Finally, in Section 4, we report results.

  20. Noble gas adsorption in two-dimensional zeolites: a combined experimental and density functional theory study

    Science.gov (United States)

    Wang, Mengen; Zhong, Jianqiang; Boscoboinik, Jorge Anibal; Lu, Deyu

    Zeolites are important industrial catalysts with porous three-dimensional structures. The catalytically active sites are located inside the pores, thus rendering them inaccessible for surface science measurements. We synthesized a two-dimensional (2D) zeolite model system, consisting of an (alumino)silicate bilayer weakly bound to a Ru (0001) surface. The 2D zeolite is suitable for surface science studies; it allows a detailed characterization of the atomic structure of the active site and interrogation of the model system during the catalytic reaction. As an initial step, we use Ar adsorption to obtain a better understanding of the atomic structure of the 2D zeolite. In addition, atomic level studies of rare gas adsorption and separation by zeolite are important for its potential application in nuclear waste sequestration. Experimental studies found that Ar atoms can be trapped inside the 2D-zeolite, raising an interesting question on whether Ar atoms are trapped inside the hexagonal prism nano-cages or at the interface between the (alumino)silicate bilayer and Ru(0001), or both. DFT calculations using van der Waals density functionals were carried out to determine the preferred Ar adsorption sites and the corresponding adsorption energies. This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science Facility, at Brookhaven National Laboratory under Contract No. DE-SC0012704.

  1. Hydrothermally stable, low-temperature NO.sub.x reduction NH.sub.3-SCR catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Narula, Chaitanya K.; Yang, Xiaofan

    2016-10-25

    A catalyst composition includes a heterobimetallic zeolite characterized by a chabazite structure loaded with copper ions and at least one trivalent metal ion other than Al.sup.3+. The catalyst composition decreases NO.sub.x emissions in diesel exhaust and is suitable for operation in a catalytic converter.

  2. Hydrothermally stable, low-temperature NO.sub.x reduction NH.sub.3-SCR catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Narula, Chaitanya K; Yang, Xiaofan

    2015-03-24

    A catalyst composition includes a heterobimetallic zeolite characterized by a chabazite structure loaded with copper ions and at least one trivalent metal ion other than Al.sup.3+. The catalyst composition decreases NO.sub.x emissions in diesel exhaust and is suitable for operation in a catalytic converter.

  3. Catalytic Dehydrogenation over Pd-Supported ZSM-5 Zeolite for o-Phenylphenol Synthesis%载钯ZSM-5分子筛催化脱氢合成邻苯基苯酚

    Institute of Scientific and Technical Information of China (English)

    蔡春; 吕春绪

    2001-01-01

    Pd-supported ZSM-5 zeolites prepared through ion exchange technique were used as a dehydrogenation catalyst for synthesis of o-phenylphenol from cyclohexanone. When Si/A1 ratio in the catalyst was 85: 1 or more, an obvious reduction in attenuation rate of catalyst activity was observed.When the Si/Al ratio was of 17 . 1 or less, polymer compounds could be formed on the surface of zeolite, that would decrease the dehydrogenation activity due to the reduction of the specific surface area of the catalyst.

  4. Synthesis of ITQ-2 zeolite under static conditions and its properties

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    Using silica gel as the precursor, MCM-22(p) was synthesized under the static conditions. Then ITQ-2 zeolite was obtained by using n-cetyltrimethylammonium bromide (CTAB) and tetrapro- pylammonium hydroxide (TPAOH) as the swelling agents to swell the pores of MCM-22(p). The ob- tained zeolite was characterized by XRD, SEM, BET, NH3-TPD. The results show that the zeolite had the best swelling when MCM-22(p):CTAB:TPAOH=1:4:1. The synthesis duration and temperature did not influence significantly the pore swelling. Except TPAOH, CTAB can also be used together with tetrabuthylammonium hydroxide (TBAOH) as the pore swelling agent. There was contribution of sur- face area and pore volume from the mesoporous pores in the ITQ-2 zeolite and it also showed weaker acidity than MCM-22. However, the ITQ-2 supported NiW catalyst showed higher activity and selec- tivity to the middle distillates in the hydrocracking of vacuum gasoil (VGO) than MCM-22 supported catalyst. This implied that the diffusion of large molecules of heavy oil in the catalyst was facilitated due to the presence of the mesoporous pores and hence higher activity and selectivity to middle dis- tillates.

  5. Estudo e caracterização da zeólita OFF Tipo T empregando diferentes fontes de silício Study and characterization of zeolite Offretite Type T employing differents silicon sources

    Directory of Open Access Journals (Sweden)

    Alessandra Caovilla

    2009-01-01

    Full Text Available Offretite T zeolite was synthesized using different source of Si (Ludox AS-30, Ludox LS-30 and Aerosil 200 Degussa. The obtained materials were characterized by different complementary techniques: XRD, textural analysis by N2 adsorption, IV, SEM and chemistry analysis. This zeolite has an intermediary structure between offretite and erionite zeolites. In all experiments offretite T phase was obtained. Offretite phase presenting better crystalility are obtained in synthesis with stirring and employing aerosil as silicon source. This zeolite presents a potencial application as catalyst for hydroisodewaxing process.

  6. Hydrodeoxygenation of fatty acid esters catalyzed by Ni on nano-sized MFI type zeolites

    Energy Technology Data Exchange (ETDEWEB)

    Schreiber, Moritz W.; Rodriguez-Niño, Daniella; Gutiérrez, Oliver Y.; Lercher, Johannes A.

    2016-01-01

    The impact of support morphology and composition on the intrinsic activity of Ni supported on MFI-type zeolite was explored in the hydrodeoxygenation of methyl stearate, tristearate, and algae oil (mixture of triglycerides). The nano-sized structure of the support (self-pillared nanosheets) is beneficial for the activity of the catalysts. Higher Ni dispersion and concomitant higher reaction rates were obtained on nano-structured supports than on zeolite with conventional morphology. Rates normalized to accessible Ni atoms (TOF), however, varied little with support morphology. Acidity of the support increases the rate of Ni-catalyzed C-O hydrogenolysis per surface metal site.

  7. Catalytic pyrolysis using UZM-39 aluminosilicate zeolite

    Science.gov (United States)

    Nicholas, Christpher P; Boldingh, Edwin P

    2013-12-17

    A new family of coherently grown composites of TUN and IMF zeotypes has been synthesized and show to be effective catalysts for catalytic pyrolysis of biomass. These zeolites are represented by the empirical formula. Na.sub.nM.sub.m.sup.n+R.sub.rQ.sub.qAl.sub1-xE.sub.xSi.sub.yO.s- ub.z where M represents zinc or a metal or metals from Group 1, Group 2, Group 3 or the lanthanide series of the periodic table, R is an A,.OMEGA.-dihalosubstituted paraffin such as 1,4-dibromobutane, Q is a neutral amine containing 5 or fewer carbon atoms such as 1-methylpyrrolidine and E is a framework element such as gallium. The process involves contacting a carbonaceous biomass feedstock with UZM-39 at pyrolysis conditions to produce pyrolysis gases comprising hydrocarbons. The catalyst catalyzes a deoxygenation reaction converting oxygenated hyrdocarbons into hydrocarbons removing the oxygen as carbon oxides and water. A portion of the pyrolysis gases is condensed to produce low oxygen biomass-derived pyrolysis oil.

  8. Catalytic pyrolysis using UZM-39 aluminosilicate zeolite

    Energy Technology Data Exchange (ETDEWEB)

    Nicholas, Christopher P; Boldingh, Edwin P

    2014-10-07

    A new family of coherently grown composites of TUN and IMF zeotypes has been synthesized and shown to be effective catalysts for catalytic pyrolysis of biomass. These zeolites are represented by the empirical formula. Na.sub.nM.sub.m.sup.n+R.sub.rQ.sub.qAl.sub.1-xE.sub.xSi.sub.yO.s- ub.z where M represents zinc or a metal or metals from Group 1, Group 2, Group 3 or the lanthanide series of the periodic table, R is an A,.OMEGA.-dihalosubstituted paraffin such as 1,4-dibromobutane, Q is a neutral amine containing 5 or fewer carbon atoms such as 1-methylpyrrolidine and E is a framework element such as gallium. The process involves contacting a carbonaceous biomass feedstock with UZM-39 at pyrolysis conditions to produce pyrolysis gases comprising hydrocarbons. The catalyst catalyzes a deoxygenation reaction converting oxygenated hydrocarbons into hydrocarbons and removing the oxygen as carbon oxides and water. A portion of the pyrolysis gases is condensed to produce low oxygen biomass-derived pyrolysis oil.

  9. Catalyst for reduction of nitrogen oxides

    Science.gov (United States)

    Ott, Kevin C.

    2010-04-06

    A Selective Catalytic Reduction (SCR) catalyst was prepared by slurry coating ZSM-5 zeolite onto a cordierite monolith, then subliming an iron salt onto the zeolite, calcining the monolith, and then dipping the monolith either into an aqueous solution of manganese nitrate and cerium nitrate and then calcining, or by similar treatment with separate solutions of manganese nitrate and cerium nitrate. The supported catalyst containing iron, manganese, and cerium showed 80 percent conversion at 113 degrees Celsius of a feed gas containing nitrogen oxides having 4 parts NO to one part NO.sub.2, about one equivalent ammonia, and excess oxygen; conversion improved to 94 percent at 147 degrees Celsius. N.sub.2O was not detected (detection limit: 0.6 percent N.sub.2O).

  10. Síntesis y caracterización de la zeolita Beta

    Directory of Open Access Journals (Sweden)

    Mahiceth Quintero

    2012-12-01

    Full Text Available Beta zeolite is normally obtained with Si/Al 5 and infinity ratios, using tetraethylammonium (TEA as templante. Important parameters in the TEA-Beta synthesis are alkali cation concentration, the type of cation used, the concentration of hydroxide, and the amount of templante, the temperature and the source of silica used. The synthesis with ratios Si:Al above 80 are generally quite difficult to achieve, but have recently been reported with all silica synthesis using TEA as templante. Their main applications are in the catalytic processes of hydrocarbon transformation (alkylation, in the inorganic membrane preparation and like “seed” in the synthesis of other zeolites. It is a microporous solid, with a unique system of channels and characteristic a chemical composition. In this work Beta zeolite was synthesized with aluminum sulfate like aluminum source. The phase identified in the pattern of X-ray diffraction obtained, coincides with the structure of the zeolite Beta.

  11. Preparation of zeolite covered cellulose fibers

    Energy Technology Data Exchange (ETDEWEB)

    Mintova, S.; Valtchev, V. [Institute of Applied Mineralogy, Sofia (Bulgaria)

    1995-12-01

    Membrane separation has proved to be an important technology in chemical industry. That is why the design of different type of zeolite containing membranes has received much attention during the last decade. Zeolite containing filters and membranes were prepared by embedding zeolite crystals with adhesive substances in the cellulose matrix. This communication discussed the preparation of zeolite containing cellulose materials by in situ crystallization. Discussed axe: (1) the effect of the vegetal fiber structure and chemical composition (2) the effect of the type of the zeolite coating; (3) the effect of the mechanical and chemical treatment of the fibers on the process of the fiber zeolite coating.

  12. A Laboratory Test Setup for in Situ Measurements of the Dielectric Properties of Catalyst Powder Samples under Reaction Conditions by Microwave Cavity Perturbation: Set up and Initial Tests

    OpenAIRE

    Markus Dietrich; Dieter Rauch; Adrian Porch; Ralf Moos

    2014-01-01

    The catalytic behavior of zeolite catalysts for the ammonia-based selective catalytic reduction (SCR) of nitrogen oxides (NOX) depends strongly on the type of zeolite material. An essential precondition for SCR is a previous ammonia gas adsorption that occurs on acidic sites of the zeolite. In order to understand and develop SCR active materials, it is crucial to know the amount of sorbed ammonia under reaction conditions. To support classical temperature-programmed desorption (TPD) experimen...

  13. Synthesis and Characterization of High Aluminum Zeolite X from Technical Grade Materials

    Directory of Open Access Journals (Sweden)

    Seyed Kamal Masoudian

    2013-06-01

    Full Text Available Zeolites are widely used as ion exchangers, adsorbents, separation materials and catalyst due to their well-tailored and highly-reproducible structures; therefore, the synthesis of zeolite from low grade resources can be interested. In the present work, high aluminum zeolite X was prepared from mixing technical grade sodium aluminate and sodium silicate solutions at temperatures between 70°C and 100°C. The synthesized zeolite X was characterized by SEM and X-ray methods according to ASTM standard procedures. The results showed that aging of the synthesis medium at the room temperature considerably increased the selectivity of zeolite X formation. On the other hand, high temperature of reaction mixture during crystallization formed zeolite A in the product; therefore, it decreased the purity of zeolite X. In addition, it was found that increasing H2O/Na2O and decreasing Na2O/SiO2 molar ratios in the reaction mixture resulted product with higher purity. © 2013 BCREC UNDIP. All rights reservedReceived: 7th January 2013; Revised: 7th April 2013; Accepted: 19th April 2013[How to Cite: Masoudian, S. K., Sadighi, S., Abbasi, A. (2013. Synthesis and Characterization of High Alu-minum Zeolite X from Technical Grade Materials. Bulletin of Chemical Reaction Engineering & Catalysis, 8 (1: 54-60. (doi:10.9767/bcrec.8.1.4321.54-60][Permalink/DOI: http://dx.doi.org/10.9767/bcrec.8.1.4321.54-60] | View in  |

  14. Methanol dehydration on carbon-based acid catalysts

    OpenAIRE

    Valero-Romero, Mª José; Calvo-Muñoz, Elisa Mª; Ruiz-Rosas, Ramiro; Rodríguez-Mirasol, José; Cordero, Tomás

    2013-01-01

    Methanol dehydration to produce dimethyl ether (DME) is an interesting process for the chemical industry since DME is an important intermediate and a promising clean alternative fuel for diesel engines. Pure or modified γ-aluminas (γ-Al2O3) and zeolites are often used as catalysts for this reaction. However, these materials usually yield non desirable hydrocarbons and undergo fast deactivation. In this work, we study the catalytic conversion of methanol over an acid carbon catalyst obtaine...

  15. Time- and space-resolved high energy operando X-ray diffraction for monitoring the methanol to hydrocarbons reaction over H-ZSM-22 zeolite catalyst in different conditions

    Science.gov (United States)

    del Campo, Pablo; Slawinski, Wojciech Andrzej; Henry, Reynald; Erichsen, Marius Westgård; Svelle, Stian; Beato, Pablo; Wragg, David; Olsbye, Unni

    2016-06-01

    The conversion of methanol to hydrocarbons (MTH) over H-ZSM-22 was studied by operando time- and space-resolved X-ray diffraction (XRD) at 370-385 °C and WHSV = 2 g/g h at the Swiss-Norwegian Beamline at ESRF. The performance of a commercial H-ZSM-22 sample was compared before and after acid-base treatment, and with and without propanol co-feed, respectively. N2 adsorption, Scanning Electron Microscopy and propyl amine desorption experiments showed that acid-base treatment led to enhanced accessibility of acid sites, mainly due to the formation of mesopores between agglomerated H-ZSM-22 crystals. The catalytic set-up allowed us to simultaneously observe the catalyst activity and unit cell volume variations by time- and space-resolved HXRD in operando conditions. The expansion of the unit cell and final flattening at different positions in the catalytic bed matched very nicely with the catalytic activity gradients. Different scenarios provided different behaviors and gave insights in the effect of morphology and co-feed process on the activity in the MTH process. This technique is the only one which has so far been able to provide direct evidence of the behavior of the species inside the catalytic reactor.

  16. Recycling of plastic materials employing zeolite and MCM-41 materials

    OpenAIRE

    Ortega, D.; L. Noreña; Aguilar, J; I. Hernández; Ramírez, V.

    2006-01-01

    We report on the catalytic and the thermal decomposition of low density polyethylene resulting in several fuel products (LP gas, gasoline, gas oil). We built a continuos, fixed-bed reaction system. We employed Ga-MCM-41, Al-MCM-41, commercial FCC Y zeolite (fresh and equilibrium) and natural mordenite as catalysts. We set the following reaction conditions: 450 °C reaction temperature, constant feed flow and 30 min reaction time at atmospheric pressure. We analyzed the gas and liquid products ...

  17. Towards a methanol economy: Zeolite catalyzed production of synthetic fuels

    DEFF Research Database (Denmark)

    Mentzel, Uffe Vie

    a commercial H-ZSM-5 zeolite impregnated with gallium and/or molybdenum is described. The object was to investigate if the presence of methanol in the feed could enhance the conversion of ethane, but in all cases the opposite is observed; the presence of methanol actually suppresses the conversion of ethane....... This observation is attributed to a stoichiometric reaction between ethane and the metal oxide species in the catalyst, leading to the oxidation of ethane to ethene, which is readily converted and incorporated into the products. Conversion of methanol, ethanol, 2-propanol, and 1 butanol to hydrocarbons over...

  18. Obtaining zeolite Y synthesized by hydrothermal treatment assisted by microwave; Obtencao de zeolita Y sintetizada atraves de tratamento hidrotermico assistido por microondas

    Energy Technology Data Exchange (ETDEWEB)

    Simoes, A.N.; Simoes, V.N.; Neiva, L.S.; Rodrigues, M.G.F.; Gama, L., E-mail: Alluskynha@hotmail.com [Universidade Federal de Campina Grande (UFCG), PB (Brazil); Oliveira, J. B.L. [Universidade Federal do Rio Grande do Norte (UFRN), Natal, RN (Brazil). Departamento de Quimica

    2011-07-01

    n search of new catalysts several man-made structures have been developed. The use of zeolites in catalysis is applied due to its ability to associate activity, selectivity and stability, the main conditions to have an effective catalyst. Thus, studies have been done on the hydrothermal synthesis of zeolites by microwave assisted, since the use of microwave radiation offers several advantages over conventional heating. In this context, this work aims to synthesis and characterization of zeolite Y via hydrothermal treatment in a microwave oven. The sample obtained was characterized by XRD, BET and SEM. XRD results showed the formation of zeolite Y in just 60 minutes. The sample showed high value of surface area, the latter being of 476.2 m² / g. The particles are agglomerated, but with a narrow distribution of size. (author)

  19. Zeolites as nanoporous, gas-sensitive materials for in situ monitoring of DeNO(x)-SCR.

    Science.gov (United States)

    Simons, Thomas; Simon, Ulrich

    2012-01-01

    In a proof-of-concept study we demonstrate in situ reaction monitoring of DeNO(x)-SCR on proton-conducting zeolites serving as catalyst and gas sensor at the same time. By means of temperature-dependent impedance spectroscopy we found that the thermally induced NH(3) desorption in H-form and in Fe-loaded zeolite H-ZSM-5 follow the same process, while a remarkable difference under DeNO(x)-SCR reaction conditions was found. The Fe-loaded catalyst shows a significantly lower onset temperature, and time-dependent measurements suggest different SCR reaction mechanisms for the two catalysts tested. These results may help in the development of catalysts for the reduction of NO(x) emissions and ammonia consumption, and provide insight into the elementary catalytic process promoting a full description of the NH(3)-SCR reaction system.

  20. STRONTIUM AS AN EFFICIENT PROMOTER FOR SUPPORTED PALLADIUM HYDROGENATION CATALYSTS

    Science.gov (United States)

    The effect of strontium promotion is studied for a series of supported palladium catalysts such as Pd/zeolite-β, Pd/Al2O3, Pd/SiO2, Pd/hydrotalcite and Pd/MgO. Strontium is found to be an effective promoter for enhancing the metal area, perce...

  1. 多级孔Hβ沸石对NiWP/Hβ-Al2 O3催化剂柴油加氢性能的影响%Influence of hierarchically mesoporous Hβzeolite on the performance of NiWP/Hβ-Al2 O3 catalysts in diesel oil hydro-upgrading

    Institute of Scientific and Technical Information of China (English)

    王海彦; 宋盼盼; 王钰佳

    2016-01-01

    Hβ-Al2 O3 composite supports were prepared through mechanically mixing Al2 O3 with hierarchically mesoporous Hβ zeolite obtained by desilication with NaOH solution; bifunctional NiWP/Hβ-Al2 O3 catalysts were then obtained by impregnation method. The composite supports and NiWP/Hβ-Al2 O3 catalysts were characterized by XRD, BET and NH3-TPD; the effect of Hβ addition on the catalytic performance of NiWP/Hβ-Al2 O3 in diesel oil hydro-upgrading was investigated in a fixed bed reactor with fluid catalytic cracking ( FCC) diesel as the feed. The results showed that by adding 15% Hβ in the Hβ-Al2 O3 composite support, NiWP/Hβ-Al2 O3 catalyst performs best in diesel oil hydro-upgrading; under 360 ℃, 8 MPa, volume space velocity of 1 . 0 h-1 and volumetric hydrogen/oil ratio of 800 , the desulfurization degree reaches 99 . 77%, the density of FCC diesel oil is decreased from 0. 927 to 0. 837 g/cm3 , while the cetane value is increased from 13 . 78 to 55 . 39 .%采用碱处理法制备多级孔Hβ沸石,以不同比例与Al2 O3混合,得到由Hβ沸石与Al2 O3组成的混合载体,再采用等体积浸渍法制备了NiWP/Hβ-Al2 O3系列催化剂。通过XRD、BET和NH3-TPD等手段对载体及催化剂进行了表征,以催化裂化柴油( FCC)为原料,在小型固定床反应器上,研究了多级孔Hβ沸石对NiWP/Hβ-Al2 O3催化剂加氢反应性能的影响。结果表明,载体中加入质量分数为15%Hβ沸石,NiWP/Hβ-Al2 O3催化剂柴油加氢性能最好;在该催化剂上,360℃、8.0 MPa、体积空速为1.0 h-1和氢油体积比800的操作条件下,脱硫率达到99.77%,催化裂化柴油的密度由0.927 g/cm3下降到0.837 g/cm3,十六烷值由13.78提高到55.39。

  2. High-Resolution Single-Molecule Fluorescence Imaging of Zeolite Aggregates within Real-Life Fluid Catalytic Cracking Particles**

    Science.gov (United States)

    Ristanović, Zoran; Kerssens, Marleen M; Kubarev, Alexey V; Hendriks, Frank C; Dedecker, Peter; Hofkens, Johan; Roeffaers, Maarten B J; Weckhuysen, Bert M

    2015-01-01

    Fluid catalytic cracking (FCC) is a major process in oil refineries to produce gasoline and base chemicals from crude oil fractions. The spatial distribution and acidity of zeolite aggregates embedded within the 50–150 μm-sized FCC spheres heavily influence their catalytic performance. Single-molecule fluorescence-based imaging methods, namely nanometer accuracy by stochastic chemical reactions (NASCA) and super-resolution optical fluctuation imaging (SOFI) were used to study the catalytic activity of sub-micrometer zeolite ZSM-5 domains within real-life FCC catalyst particles. The formation of fluorescent product molecules taking place at Brønsted acid sites was monitored with single turnover sensitivity and high spatiotemporal resolution, providing detailed insight in dispersion and catalytic activity of zeolite ZSM-5 aggregates. The results point towards substantial differences in turnover frequencies between the zeolite aggregates, revealing significant intraparticle heterogeneities in Brønsted reactivity. PMID:25504139

  3. Green acetylation of solketal and glycerol formal by heterogeneous acid catalysts to form a biodiesel fuel additive.

    Science.gov (United States)

    Dodson, Jennifer R; Leite, Thays d C M; Pontes, Nathália S; Peres Pinto, Bianca; Mota, Claudio J A

    2014-09-01

    A glut of glycerol has formed from the increased production of biodiesel, with the potential to integrate the supply chain by using glycerol additives to improve biodiesel properties. Acetylated acetals show interesting cold flow and viscosity effects. Herein, a solventless heterogeneously catalyzed process for the acetylation of both solketal and glycerol formal to new products is demonstrated. The process is optimized by studying the effect of acetylating reagent (acetic acid and acetic anhydride), reagent molar ratios, and a variety of commercial solid acid catalysts (Amberlyst-15, zeolite Beta, K-10 Montmorillonite, and niobium phosphate) on the conversion and selectivities. High conversions (72-95%) and selectivities (86-99%) to the desired products results from using acetic anhydride as the acetylation reagent and a 1:1 molar ratio with all catalysts. Overall, there is a complex interplay between the solid catalyst, reagent ratio, and acetylating agent on the conversion, selectivities, and byproducts formed. The variations are discussed and explained in terms of reactivity, thermodynamics, and reaction mechanisms. An alternative and efficient approach to the formation of 100% triacetin involves the ring-opening, acid-catalyzed acetylation from solketal or glycerol formal with excesses of acetic anhydride.

  4. Zeolite H-USY for the production of lactic acid and methyl lactate from C-3-sugars

    DEFF Research Database (Denmark)

    West, R.M.; Holm, Martin Spangsberg; Shunmugavel, Saravanamurugan

    2010-01-01

    Lactic acid is an interesting platform chemical with many promising applications. This includes the use as a building block for the production of biodegradable plastics and environmentally friendly solvents. A study of the liquid-phase conversion of the triose-sugars, glyceraldehyde...... and dihydroxyacetone directly to methyl lactate and lactic acid catalyzed by inexpensive commercially available zeolites is presented. One particular zeolite, H-USY (Si/Al = 6) is shown to be quite active with near quantitative yields for this isomerization. Deactivation of the H-USY-zeolite was studied by correlating...... the catalytic activity to data obtained by TPO, XRD, N-2-sorption, and NH3-TPD on fresh and used catalysts. Coking and irreversible framework damage occurs when lactic acid is produced under aqueous conditions. In methanol, methyl lactate is produced and catalyst deactivation is suppressed. Additionally...

  5. Insecticide Effect of Zeolites on the Tomato Leafminer Tuta absoluta (Lepidoptera: Gelechiidae)

    Science.gov (United States)

    De Smedt, Caroline; Van Damme, Veerle; De Clercq, Patrick; Spanoghe, Pieter

    2016-01-01

    (1) Background: The tomato leafminer Tuta absoluta (Lepidoptera: Gelechiidae) is a key tomato insect pest. At present, it is considered to be a serious threat in various countries in Europe, North Africa, and Middle East. The extensive use and the developed resistance of T. absoluta to spinosad causes some concern, which leads to the need for alternative products. (2) Materials and Methods: Several laboratory experiments were conducted to investigate the ovicidal properties of a zeolite particle film on T. absoluta. The toxicity of three different zeolites and six zeolite formulations to T. absoluta eggs and larvae was determined using different exposure methods. (3) Results: In general, the formulated zeolites yielded higher egg and larvae mortality values, especially when the zeolite particle film was residually applied. Notable differences in mortality rates from exposure to zeolites compared to other products, such as kaolin, its formulated product Surround, and the insecticide spinosad, were observed. Kaolin and Surround exhibited little or no effect for both application methods, while the hatch rate was reduced by 95% when spinosad was applied topically. Spinosad yielded egg and larvae mortality rates of 100% for both application methods. Additionally, increased oviposition activity was observed in adults exposed to the wettable powder (WP) formulations. These WP formulations increased egg deposition, while Surround and spinosad elicited a negative oviposition response. (4) Conclusions: It can be derived that the tested products, zeolites BEA (Beta polymorph A), FAU (Faujasite), LTA (Linde type A), and their formulations, had no real insecticidal activity against the eggs of T. absoluta. Nevertheless, egg exposure to zeolites seemed to affect the development process by weakening the first instar larvae and increasing their mortality. Subsequently, based on the choice test, no significant difference was observed between the number of eggs laid on the treated

  6. Insecticide Effect of Zeolites on the Tomato Leafminer Tuta absoluta (Lepidoptera: Gelechiidae

    Directory of Open Access Journals (Sweden)

    Caroline De Smedt

    2016-12-01

    Full Text Available (1 Background: The tomato leafminer Tuta absoluta (Lepidoptera: Gelechiidae is a key tomato insect pest. At present, it is considered to be a serious threat in various countries in Europe, North Africa, and Middle East. The extensive use and the developed resistance of T. absoluta to spinosad causes some concern, which leads to the need for alternative products. (2 Materials and Methods: Several laboratory experiments were conducted to investigate the ovicidal properties of a zeolite particle film on T. absoluta. The toxicity of three different zeolites and six zeolite formulations to T. absoluta eggs and larvae was determined using different exposure methods. (3 Results: In general, the formulated zeolites yielded higher egg and larvae mortality values, especially when the zeolite particle film was residually applied. Notable differences in mortality rates from exposure to zeolites compared to other products, such as kaolin, its formulated product Surround, and the insecticide spinosad, were observed. Kaolin and Surround exhibited little or no effect for both application methods, while the hatch rate was reduced by 95% when spinosad was applied topically. Spinosad yielded egg and larvae mortality rates of 100% for both application methods. Additionally, increased oviposition activity was observed in adults exposed to the wettable powder (WP formulations. These WP formulations increased egg deposition, while Surround and spinosad elicited a negative oviposition response. (4 Conclusions: It can be derived that the tested products, zeolites BEA (Beta polymorph A, FAU (Faujasite, LTA (Linde type A, and their formulations, had no real insecticidal activity against the eggs of T. absoluta. Nevertheless, egg exposure to zeolites seemed to affect the development process by weakening the first instar larvae and increasing their mortality. Subsequently, based on the choice test, no significant difference was observed between the number of eggs laid on

  7. Zeolites on Mars: Possible environmental indicators in soils and sediments

    Science.gov (United States)

    Ming, D. W.; Gooding, J. L.

    1988-01-01

    Weathering products should serve as indicators of weathering environments and may provide the best evidence of the nature of climate change on Mars. No direct mineralogical measurements of Martian regolith were performed by the Viking missions, but the biology and X-ray fluorescence experiments provided some information on the physiochemical properties of Martian regolith. Most post-Viking studies of candidate weathering products have emphasized phyllosilicates and Fe-oxides; zeolites are potentially important, but overlooked, candidate Martian minerals. Zeolites would be important on Mars for three different reasons. First, they are major sinks of atmospheric gases and, per unit mass, are stronger and more efficient sorbents than are phyllosilicates. Secondly, they can be virtually unique sorbents and shelters for organic compounds and possible catalysts for organic-based reactions. Finally, their exchangeable ions are good indicators of the chemical properties of solutions with which they have communicated. Accordingly, the search for information on past compositions of the Martian atmosphere and hydrosphere should find zeolites to be rich repositories.

  8. Influence of the metal substrate properties on kinetics of zeolite film formation

    Energy Technology Data Exchange (ETDEWEB)

    Valtchev, V.; Mintova, S.; Konstantinov, L. [Institute of Applied Mineralogy, Sofia (Bulgaria)

    1995-12-01

    The main stages of film formation of the zeolites A. Y and silicalite-1 on differently pretreated cooper substrates is considered from the viewpoint of the film morphology. The molecular sieves crystallization on metal substrate. and microporous modules has extensively studied during last years due to their potential in designing chemical sensors, gas separators, catalysts. etc. The gel chemical composition. the substrate surface structure and its position in the reactor influence considerably the zeolite film formation. The kinetics of film formation is by no means a simple subject to study and its detailed characterization requires an optimal choice of parameters. In this work we consider some kinetics aspects of the deposition of films of zeolites A, Y and silicalite-1 on differently pretreated cooper substrates.

  9. A new metal exchanged zeolite for a present environmental problem. An in-situ XAS study

    Science.gov (United States)

    Alonso-Escobar, C.; Franch-Martí, C.; Palomares, A. E.; Rey, F.; Guilera, G.

    2013-04-01

    The medium pore zeolite, TNU-9, is prepared and studied for the selective catalytic reduction (SCR) of NO using C3H8 as the reducing agent. The catalytic activity of TNU-9 zeolites for the SCR is comparable to other known highly active zeolites but with the advantage of TNU-9 of having almost the same catalytic performance in the presence of H2O during reaction. The nature and behaviour of Cu and Co active sites contained in the TNU-9 catalysts have been studied under operation conditions using X-ray Absorption Spectroscopy (XAS) to understand the key parameters controlling the performance of this reaction.1 It was found that the well dispersed Cu and Co centres need to be in a mixed valence state to obtain good catalytic results for the SCR and that the catalytic performance is related to the topology of the TNU-9 itself.

  10. Selective catalytic reduction of nitric oxide by ammonia over Cu-exchanged Cuban natural zeolites

    Energy Technology Data Exchange (ETDEWEB)

    Moreno-Tost, Ramon; Santamaria-Gonzalez, Jose; Rodriguez-Castellon, Enrique; Jimenez-Lopez, Antonio [Departamento de Quimica Inorganica, Cristalografia y Mineralogia, Facultad de Ciencias, Unidad Asociada del Instituto de Catalisis y Petroleoquimica, CSIC, Universidad de Malaga, Campus de Teatinos, 29071 Malaga (Spain); Autie, Miguel A.; Glacial, Marisol Carreras [Centro Nacional de Investigaciones Cientificas, Ciudad de la Habana, La Habana (Cuba); Gonzalez, Edel [Instituto Superior Pedagogico ' Enrique Jose Varona' , La Habana (Cuba); Pozas, Carlos De las [Centro de Gerencia de Programas y Proyectos Priorizados, La Habana (Cuba)

    2004-07-15

    The catalytic selective reduction of NO over Cu-exchanged natural zeolites (mordenite (MP) and clinoptilolite (HC)) from Cuba using NH{sub 3} as reducing agent and in the presence of excess oxygen was studied. Cu(II)-exchanged zeolites are very active catalysts, with conversions of NO of 95%, a high selectivity to N{sub 2} at low temperatures, and exhibiting good water tolerance. The chemical state of the Cu(II) in exchanged zeolites was characterized by H{sub 2}-TPR and XPS. Cu(II)-exchanged clinoptilolite underwent a severe deactivation in the presence of SO{sub 2}. However, Cu(II)-exchanged mordenite not only maintained its catalytic activity, but even showed a slight improvement after 20h of reaction in the presence of 100ppm of SO{sub 2}.

  11. A convenient synthesis of 1,5-diarylpyrazoles from Baylis-Hillman adducts using HY-zeolite

    Institute of Scientific and Technical Information of China (English)

    Mohammad; Nikpassand; Manouchehr; Mamaghani; Mohammad; Ali; Zanjanchi; Nosrat; Olah; Mahmoodi; Massomeh; Mirzaeinejad

    2010-01-01

    A facile and convenient protocol was developed for the synthesis of 1,5-diarylpyrazoles using Baylis-Hillman adducts in the presence of HY-zeolite as an efficient recyclable heterogeneous catalyst in reasonable reaction times(1.5-2.5 h) and high yields (78-90%).

  12. Confirmation of Isolated Cu2+ Ions in SSZ-13 Zeolite as Active Sites in NH3-Selective Catalytic Reduction

    NARCIS (Netherlands)

    Deka, U.; Juhin, A.F.; Eilertsen, E.A.; Emerich, H.; Green, M.A.; Korhonen, S.T.; Weckhuysen, B.M.; Beale, A.M.

    2012-01-01

    NH3-Selective Catalytic Reduction (NH3-SCR) is a widely used technology for NOx reduction in the emission control systems of heavy duty diesel vehicles. Copper-based ion exchanged zeolites and in particular Cu-SSZ-13 (CHA framework) catalysts show both exceptional activity and hydrothermal stability

  13. Spectra of carbanions formed from allyl cyanide during isomerization in zeolite NaY-FAU with strong basic sites

    Science.gov (United States)

    Hannus, István; Förster, Horst; Tasi, Gyula; Kiricsi, Imre; Molnár, Árpád

    1995-03-01

    Double bond isomerization of allyl cyanide to crotononitrile over a basic zeolite catalyst was monitored by IR and UV-VIS spectroscopy in order to get information on the surface intermediates involved. Due to the spectral changes the occurence of a carbanionic intermediate seems to be highly probable characterized by an absorption at 400 nm.

  14. Ultrasound assisted, ruthenium-exchanged FAU-Y zeolite catalyzed alkylation of indoles with epoxides under solvent free conditions.

    Science.gov (United States)

    Khorshidi, Alireza

    2012-05-01

    Ruthenium-exchanged FAU-Y zeolite (RuY) was used as a recyclable catalyst for regioselective ring-opening of epoxides with indoles under irradiation of sonic waves. It was found that a solvent free process, under the above mentioned conditions provides good yields of the desired 3-alkylated indole derivatives.

  15. Simultaneous coking and dealumination of zeolite H-ZSM-5 during the transformation of chloromethane into olefins

    NARCIS (Netherlands)

    Ibanez, M.; Gamero, M.; Ruiz-Martinez, J.; Weckhuysen, B. M.; Aguayo, A. T.; Bilbao, J.; Castano, P.

    2016-01-01

    The deactivation pathways of a zeolite H-ZSM-5 catalyst containing bentonite and alpha-Al2O3 as binder material have been studied during the transformation of chloromethane into light olefins, which is considered as a possible step to valorize methane from natural gas. The reactions have been carrie

  16. Metal immobilization in soils using synthetic zeolites

    NARCIS (Netherlands)

    Osté, L.A.; Lexmond, T.M.; Riemsdijk, van W.H.

    2002-01-01

    In situ immobilization of heavy metals in contaminated soils is a technique to improve soil quality. Synthetic zeolites are potentially useful additives to bind heavy metals. This study selected the most effective zeolite in cadmium and zinc binding out of six synthetic zeolites (mordenite-type, fau

  17. Method of producing zeolite encapsulated nanoparticles

    DEFF Research Database (Denmark)

    2015-01-01

    The invention therefore relates to a method for producing zeolite, zeolite-like or zeotype encapsulated metal nanoparticles, the method comprises the steps of: 1) Adding one or more metal precursors to a silica or alumina source; 2) Reducing the one or more metal precursors to form metal nanopart......The invention therefore relates to a method for producing zeolite, zeolite-like or zeotype encapsulated metal nanoparticles, the method comprises the steps of: 1) Adding one or more metal precursors to a silica or alumina source; 2) Reducing the one or more metal precursors to form metal...... nanoparticles on the surface of the silica or alumina source; 3) Passing a gaseous hydrocarbon, alkyl alcohol or alkyl ether over the silica or alumina supported metal nanoparticles to form a carbon template coated zeolite, zeolite-like or zeotype precursor composition; 4a) Adding a structure directing agent...... to the carbon template coated zeolite, zeolite-like or zeotype precursor composition thereby creating a zeolite, zeolite-like or zeotype gel composition; 4b) Crystallising the zeolite, zeolite-like or zeotype gel composition by subjecting said composition to a hydrothermal treatment; 5) Removing the carbon...

  18. Stability and activity of doped transition metal zeolites in the hydrothermal processing

    Directory of Open Access Journals (Sweden)

    Thomas François Robin

    2015-12-01

    Full Text Available This study investigates the stability and activity of HZSM-5 doped with metals such as molybdenum, nickel, copper and iron in under hydrothermal conditions used for the direct liquefaction of microalgae. Catalysts have been prepared by ion exchange techniques, and MoZSM-5 was also prepared by wet incipient impregnation for comparison. Hydrothermal liquefaction is considered as a potential route to convert microalgae into a sustainable fuel. One of the drawbacks of this process is that the bio-crude produced contains significant levels of nitrogen and oxygen compounds which have an impact on the physical and chemical propriety of the fuel. Heterogeneous catalysts have been shown to improve the quality of the bio-crude by reducing nitrogen and oxygen contents. Zeolites, such as HZSM-5, are strong candidates due to their low cost compared to noble metal catalysts but their stability and activity under hydrothermal conditions is not well understood. The stability of the catalysts has been determined under hydrothermal conditions at 350 °C. Catalysts have been characterised before and after treatment using XRD, BET physisorption and STEM microscopy. Metal leaching was determined by analysis of the water phase following hydrothermal treatment. The inserted cation following ion-exchange can influence the physical properties of HZSM-5 for example molybdenum improves the crystallinity of the zeolite. In general, metal doped zeolites were relatively stable under subcritical water. Activity of the catalysts for processing lipids, protein and microalgae has been assessed. Four feedstocks were selected: sunflower oil, soya proteins, Chlorella and P. ellipsoidea. The catalysts exhibited greater activity towards converting lipids for example MoZSM-5 enhanced the formation of aromatic compounds. NiZSM-5 and CuZSM-5 were observed to be more efficient for deoxygenation.

  19. Photocatalysis of fenoxycarb over silver-modified zeolites.

    Science.gov (United States)

    Ahern, John; Kanan, Sofian; Sara, Ziad; Job, Thomas; Alnaizy, Raafat; Abu Farha, Nedal; Patterson, Howard

    2015-03-01

    Two samples of silver doped into zeolite Y were prepared and characterized. ICP and SEM-EDS analysis indicate that the AgY1 sample contains twice the amount of silver compared to the AgY2 sample. Solid state luminescence spectroscopy shows variations in the emission modes of the site-selective luminescence where various luminophores might be excited upon selecting the proper excitation energy. The selected material effectively decomposed the pesticide fenoxycarb in aqueous solution. The photodecomposition of fenoxycarb reached 80 % upon irradiation for 60 min in the presence of the AgY1 catalyst. 2-(4-Phenoxy-phenoxy)ethyl] carbamic acid (1) and 1-amine-2-(phenoxy-4-ol) ethane (2) were identified as products for both uncatalyzed solution and the catalyzed fenoxycarb with AgY2 catalyst. Whereas, compound (2) was the only product identified in the catalyzed reaction with AgY1.

  20. Unstitching the nanoscopic mystery of zeolite crystal formation.

    Science.gov (United States)

    Brent, Rhea; Cubillas, Pablo; Stevens, Sam M; Jelfs, Kim E; Umemura, Ayako; Gebbie, James T; Slater, Ben; Terasaki, Osamu; Holden, Mark A; Anderson, Michael W

    2010-10-06

    A molecular-scale understanding of crystal growth is critical to the development of important materials such as pharmaceuticals, semiconductors and catalysts. Only recently has this been possible with the advent of atomic force microscopy that permits observation of nanoscopic features on solid surfaces under a liquid or solution environment. This allows in situ measurement of important chemical transformations such as crystal growth and dissolution. Further, the microscope can access not only an accurate height measurement of surface topography, important to deduce structural elements, but also the forces involved during nanoscopic processes. We have discovered that it is possible to use these features to "illuminate" critical nanoscopic chemical events at crystal surfaces and at the same time extract the associated energies and unstitch the details of the stepwise mechanism of growth and dissolution. This approach has been developed using nanoporous crystals of the heterogeneous catalyst zeolite L; however, in principle the approach could be adapted to many crystal growth problems.

  1. Synthesis, characterization and catalytic activity of indium substituted nanocrystalline Mobil Five (MFI) zeolite

    Energy Technology Data Exchange (ETDEWEB)

    Shah, Kishor Kr. [Department of Chemistry, ADP College, Nagaon, Assam 782002 (India); Nandi, Mithun [Department of Chemistry, Gauhati University, Guwahati, Assam 781014 (India); Talukdar, Anup K., E-mail: anup_t@sify.com [Department of Chemistry, Gauhati University, Guwahati, Assam 781014 (India)

    2015-06-15

    Highlights: • In situ modification of the MFI zeolite by incorporation of indium. • The samples were characterized by XRD, FTIR, TGA, UV–vis (DRS), SAA, EDX and SEM. • The incorporation of indium was confirmed by XRD, FT-IR, UV–vis (DRS), EDX and TGA. • Hydroxylation of phenol reaction was studied on the synthesized catalysts. - Abstract: A series of indium doped Mobil Five (MFI) zeolite were synthesized hydrothermally with silicon to aluminium and indium molar ratio of 100 and with aluminium to indium molar ratios of 1:1, 2:1 and 3:1. The MFI zeolite phase was identified by XRD and FT-IR analysis. In XRD analysis the prominent peaks were observed at 2θ values of around 6.5° and 23° with a few additional shoulder peaks in case of all the indium incorporated samples suggesting formation of pure phase of the MFI zeolite. All the samples under the present investigation were found to exhibit high crystallinity (∼92%). The crystallite sizes of the samples were found to vary from about 49 to 55 nm. IR results confirmed the formation of MFI zeolite in all cases showing distinct absorbance bands near 1080, 790, 540, 450 and 990 cm{sup −1}. TG analysis of In-MFI zeolites showed mass losses in three different steps which are attributed to the loss due to adsorbed water molecules and the two types TPA{sup +} cations. Further, the UV–vis (DRS) studies reflected the position of the indium metal in the zeolite framework. Surface area analysis of the synthesized samples was carried out to characterize the synthesized samples The analysis showed that the specific surface area ranged from ∼357 to ∼361 m{sup 2} g{sup −1} and the pore volume of the synthesized samples ranged from 0.177 to 0.182 cm{sup 3} g{sup −1}. The scanning electron microscopy studies showed the structure of the samples to be rectangular and twinned rectangular shaped. The EDX analysis was carried out for confirmation of Si, Al and In in zeolite frame work. The catalytic activities of

  2. Synthesis Strategies for Ultrastable Zeolite GIS Polymorphs as Sorbents for Selective Separations

    Energy Technology Data Exchange (ETDEWEB)

    Oleksiak, Matthew D. [Department of Chemical and Biomolecular Engineering, University of Houston, Houston TX 77204 USA; Ghorbanpour, Arian [Department of Chemical and Biomolecular Engineering, University of Houston, Houston TX 77204 USA; Conato, Marlon T. [Department of Chemical and Biomolecular Engineering, University of Houston, Houston TX 77204 USA; Institute of Chemistry, University of the Philippines, Diliman Quezon City 1101 Philippines; McGrail, B. Peter [Applied Functional Materials, Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland WA 99354 USA; Grabow, Lars C. [Department of Chemical and Biomolecular Engineering, University of Houston, Houston TX 77204 USA; Motkuri, Radha Kishan [Applied Functional Materials, Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland WA 99354 USA; Rimer, Jeffrey D. [Department of Chemical and Biomolecular Engineering, University of Houston, Houston TX 77204 USA

    2016-10-05

    Designing nanoporous zeolites with tunable physicochemical properties can substantially impact their performance in commercial applications spanning diverse areas such as adsorption, separations, catalysis, and drug delivery. Zeolite synthesis typically requires the use of an organic structure-directing agent to facilitate the formation of crystals with specific pore size and topology. Attempts to remove organics from syntheses to achieve commercially-viable methods of preparing zeolites often lead to the formation of unwanted crystal polymorphs (i.e., impurities). Here, we present an organic-free synthesis of the small-pore zeolite P (GIS framework topology) that can be selectively tailored to produce two pure polymorphs: P1 and P2. To this end, we developed kinetic phase diagrams that identify synthesis compositions leading to the formation of GIS (P1 and P2), as well as their structural analogues MER and PHI. Using a combination of adsorption measurements and density functional theory (DFT) calculations, we also show that both GIS polymorphs are highly selective adsorbents for H2O relative to other light gases (e.g,, H2, N2, CO2). These studies highlight the potential application of GIS materials for dehydration processes, while our findings also refute prior theoretical studies postulating that GIS-type zeolites are excellent materials for CO2 separation/sequestration. Moreover, there is an impetus for discovering novel small-pore zeolites that are shape-selective catalysts for the production of value-added chemicals (e.g., light olefins); thus, our discovery of more thermally-stable P2 opens new avenues for exploring the potential role of this material as a high-performance catalyst.

  3. A transmission infrared cell design for temperature-controlled adsorption and reactivity studies on heterogeneous catalysts

    Science.gov (United States)

    Cybulskis, Viktor J.; Harris, James W.; Zvinevich, Yury; Ribeiro, Fabio H.; Gounder, Rajamani

    2016-10-01

    A design is presented for a versatile transmission infrared cell that can interface with an external vacuum manifold to undergo in situ gas treatments and receive controlled doses of various adsorbates and probe molecules, allowing characterization of heterogeneous catalyst surfaces in order to identify and quantify active sites and adsorbed surface species. Critical design characteristics include customized temperature control for operation between cryogenic and elevated temperatures (100-1000 K) and modified Cajon fittings for operation over a wide pressure range (10-2-103 Torr) that eliminates the complications introduced when using sealants or flanges to secure cell windows. The customized, hand-tightened Cajon fittings simplify operation of the cell compared to previously reported designs, because they allow for rapid cell assembly and disassembly and, in turn, replacement of catalyst samples. In order to validate the performance of the cell, transmission infrared spectroscopic experiments are reported to characterize the Brønsted and Lewis acid sites present in H-beta and H-mordenite zeolites using cryogenic adsorption of CO (<150 K).

  4. Study on molecular sieve catalyst on catalytic properties of phenol and isopropanol alkylation%分子筛催化剂对苯酚异丙醇烷基化反应催化性能的研究

    Institute of Scientific and Technical Information of China (English)

    张丽; 赵娜; 王莹莹

    2013-01-01

    Alkylation of phenol with isopropanol was carried out on three different kinds of molecular sieve catalysts, MCM-56, ZSM-22 and Beta zeolite. X-ray diffraction and NH3-TPD were used to characterize the three zeolite.The remit showd that the weak acid sites of the catalysts favor o-isopropyl phenol and the strong acad sites favor p-isopropyl phenol.%本文研究了用MCM-56、ZSM-22、Beta分子筛作催化剂催化苯酚异丙醇烷基化反应的催化性能.用X射线衍射、氨程序升温脱附两种表征方法对3种分子筛进行了表征.实验表明:当分子筛具有弱酸性位时易于邻异丙基苯酚的生成,具有强酸性位时易于对异丙基苯酚的生成.

  5. Confinement effect and synergistic function of H-ZSM-5/Cu-ZnO-Al2O3 capsule catalyst for one-step controlled synthesis.

    Science.gov (United States)

    Yang, Guohui; Tsubaki, Noritatsu; Shamoto, Jun; Yoneyama, Yoshiharu; Zhang, Yi

    2010-06-16

    Dimethyl ether (DME) is an industrially important intermediate, as well as a promising clean fuel, but the effective production through traditionally consecutive steps from syngas to methanol and then to DME has been hindered by the poorly organized structure of the conventional physical mixture catalyst. Here, a novel zeolite capsule catalyst possessing a core-shell structure (millimeter-sized core catalyst and micrometer-sized acidic zeolite shell) was proposed initially through a well-designed aluminum migration method using the core catalyst as the aluminum resource and for the first time was applied to accomplish the DME direct synthesis from syngas. The selectivity of the expected DME on this zeolite capsule catalyst strikingly exceeded that of the hybrid catalyst prepared by the traditional mixing method, while maintaining the near-zero formation of the unexpected alkanes byproduct. The preliminary methanol synthesis reaction on the core catalyst and the following DME formation from methanol inside the zeolite shell cooperated concertedly and promoted mutually. This zeolite capsule catalyst with a synergetic confinement core-shell structure can be used to efficiently realize the combination of two and more sequential reactions with many synergistic effects.

  6. Benzene hydrogenation catalysed by molybdenum carbide supported on Y zeolite; Hidrogenacao de benzeno catalisada por especies do tipo carbeto de molibdenio suportado em zeolita Y

    Energy Technology Data Exchange (ETDEWEB)

    Rocha, Angela Sanches; Faro Junior, Arnaldo da Costa [Universidade Federal, Rio de Janeiro, RJ (Brazil). Inst. de Quimica. Dept. de Fisico-Quimica]. E-mail: asrocha@iq.ufrj.br; farojr@iq.ufrj.br; Silva, Victor Teixeira da [Instituto Militar de Engenharia (IME), Rio de Janeiro, RJ (Brazil). Dept. de Engenharia Quimica]. E-mail: dasilva@aquarius.ime.eb.br

    2003-07-01

    Besides increasingly severe environmental legislation that limits the amount of aromatic hydrocarbons present in diesel fuels , improvement of the cetane number stimulates the development of hydrodesaromatization (HDA) catalysts. The present work investigates zeolite-supported molybdenum carbide catalysts , as an alternative for deep HDA. The transition metal carbides display catalytic activity similar to that of the noble metals catalysts used for this purpose, but they show larger thiotolerance, and have a lower price. Molybdenum carbide supported on Y zeolite with different silica/alumina ratios (SAR) and sodium contents were prepared starting from Mo(CO){sub 6} adsorbed on the zeolites and decomposed under different gaseous atmospheres, at high temperatures. The obtained materials were tested in benzene hydrogenation at 90 deg C, showing significant activity at atmospheric pressure, which characterizes the formation of carbides species. Strong dependence of the activity of the catalysts was also observed in relation to SAR and to the quantity of sodium of the zeolite supports. FTIR results show that the presence of protons in the zeolites dis favors the formation active molybdenum species. (author)

  7. Generation of basic centers in high-silica zeolites and their application in gas-phase upgrading of bio-oil.

    Science.gov (United States)

    Keller, Tobias C; Rodrigues, Elodie G; Pérez-Ramírez, Javier

    2014-06-01

    High-silica zeolites have been reported recently as efficient catalysts for liquid- and gas-phase condensation reactions because of the presence of a complementary source of basicity compared to Al-rich basic zeolites. Herein, we describe the controlled generation of these active sites on silica-rich FAU, BEA, and MFI zeolites. Through the application of a mild base treatment in aqueous Na2CO3, alkali-metal-coordinating defects are generated within the zeolite whereas the porous properties are fully preserved. The resulting catalysts were applied in the gas-phase condensation of propanal at 673 K as a model reaction for the catalytic upgrading of pyrolysis oil, for which an up to 20-fold increased activity compared to the unmodified zeolites was attained. The moderate basicity of these new sites leads to a coke resistance superior to traditional base catalysts such as CsX and MgO, and comparable activity and excellent selectivity is achieved for the condensation pathways. Through strategic acid and base treatments and the use of magic-angle spinning NMR spectroscopy, the nature of the active sites was investigated, which supports the theory of siloxy sites as basic centers. This contribution represents a key step in the understanding and design of high-silica base catalysts for the intermediate deoxygenation of crude bio-oil prior to the hydrotreating step for the production of second-generation biofuels.

  8. Zeolite-dye micro lasers

    CERN Document Server

    Vietze, U; Laeri, F; Ihlein, G; Schüth, F; Limburg, B; Abraham, M

    1998-01-01

    We present a new class of micro lasers based on nanoporous molecular sieve host-guest systems. Organic dye guest molecules of 1-Ethyl-4-(4-(p-Dimethylaminophenyl)-1,3-butadienyl)-pyridinium Perchlorat were inserted into the 0.73-nm-wide channel pores of a zeolite AlPO$_4$-5 host. The zeolitic micro crystal compounds where hydrothermally synthesized according to a particular host-guest chemical process. The dye molecules are found not only to be aligned along the host channel axis, but to be oriented as well. Single mode laser emission at 687 nm was obtained from a whispering gallery mode oscillating in a 8-$\\mu$m-diameter monolithic micro resonator, in which the field is confined by total internal reflection at the natural hexagonal boundaries inside the zeolitic microcrystals.

  9. Zeolite synthesis: an energetic perspective.

    Science.gov (United States)

    Zwijnenburg, Martijn A; Bromley, Stefan T

    2010-11-21

    Taking |D(H(2)O)(x)|[AlSiO(4)] based materials (where D is Li, Na, K, Rb or Cs) as an archetypal aluminosilicate system, we use accurate density functional theory calculations to demonstrate how the substitution of silicon cations in silica, with pairs of aluminium and (alkali metal) cations, changes the energetic ordering of different competing structure-types. For large alkali metal cations we further show that the formation of porous aluminosilicate structures, the so-called zeolites, is energetically favored. These findings unequivocally demonstrate that zeolites can be energetic preferred reaction products, rather than being kinetically determined, and that the size of the (hydrated) cations in the pore, be it inorganic or organic, is critical for directing zeolite synthesis.

  10. Discovery of optimal zeolites for challenging separations and chemical conversions through predictive materials modeling

    Science.gov (United States)

    Siepmann, J. Ilja; Bai, Peng; Tsapatsis, Michael; Knight, Chris; Deem, Michael W.

    2015-03-01

    Zeolites play numerous important roles in modern petroleum refineries and have the potential to advance the production of fuels and chemical feedstocks from renewable resources. The performance of a zeolite as separation medium and catalyst depends on its framework structure and the type or location of active sites. To date, 213 framework types have been synthesized and >330000 thermodynamically accessible zeolite structures have been predicted. Hence, identification of optimal zeolites for a given application from the large pool of candidate structures is attractive for accelerating the pace of materials discovery. Here we identify, through a large-scale, multi-step computational screening process, promising zeolite structures for two energy-related applications: the purification of ethanol beyond the ethanol/water azeotropic concentration in a single separation step from fermentation broths and the hydroisomerization of alkanes with 18-30 carbon atoms encountered in petroleum refining. These results demonstrate that predictive modeling and data-driven science can now be applied to solve some of the most challenging separation problems involving highly non-ideal mixtures and highly articulated compounds. Financial support from the Department of Energy Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DE-FG02-12ER16362 is gratefully acknowledged.

  11. Transition phases of zeolite Faujasite type to Sodalite by thermal treatment

    Directory of Open Access Journals (Sweden)

    Katia K. Kaminishikawahara

    2015-10-01

    Full Text Available The zeolites can have several functions as catalysts (biofuel production and molecular sieves (treatment of contaminated areas. This study aims to characterize the zeolites obtained in the transition of a Faujasite like zeolite into a Sodalite, when submitted to different thermal treatment times. The synthesized zeolites were characterized by X-ray diffraction where the crystalline phases were identified: Faujasite, Sodalite, SiO2 and amorphous material. The 4 hours heat treatment produces zeolite crystal structure similar to Faujasite, having basic sites, surface area of 552.7 m2 g-1 , and pore volume of 0.3391 cm3 g-1. With increasing time of heat treatment was observed the transition to the Sodalite phase witch containing 0.277 mmol g-1 of basic active sites with surface area of 11.38 m2 g-1 and pore volume of 0.0651 cm3 g-1. By the Rietveld method was identified and quantified the presence of Sodalite and Hidrossodalite in samples with 24 and 30 hours of reaction times.

  12. Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature.

    Science.gov (United States)

    Narsimhan, Karthik; Iyoki, Kenta; Dinh, Kimberly; Román-Leshkov, Yuriy

    2016-06-22

    The direct catalytic conversion of methane to liquid oxygenated compounds, such as methanol or dimethyl ether, at low temperature using molecular oxygen is a grand challenge in C-H activation that has never been met with synthetic, heterogeneous catalysts. We report the first demonstration of direct, catalytic oxidation of methane into methanol with molecular oxygen over copper-exchanged zeolites at low reaction temperatures (483-498 K). Reaction kinetics studies show sustained catalytic activity and high selectivity for a variety of commercially available zeolite topologies under mild conditions (e.g., 483 K and atmospheric pressure). Transient and steady state measurements with isotopically labeled molecules confirm catalytic turnover. The catalytic rates and apparent activation energies are affected by the zeolite topology, with caged-based zeolites (e.g., Cu-SSZ-13) showing the highest rates. Although the reaction rates are low, the discovery of catalytic sites in copper-exchanged zeolites will accelerate the development of strategies to directly oxidize methane into methanol under mild conditions.

  13. Surface chemical modification of zeolites and their catalytic performance for naphthalene alkylation

    Institute of Scientific and Technical Information of China (English)

    张铭金; 郑安民; 邓风; 岳勇; 叶朝辉

    2003-01-01

    Zeolitesβ, Y and mordenite are modified with organic and inorganic cupric salts using a liquid phase deposit method, and their catalytic performance and the dispersion states of copper on the zeolites are characterized by using naphthalene isopropylation reaction and 129Xe NMR, respectively. The experimental results indicate that naphthalene conversion on the catalysts decreases in the order of HY>Hβ>HMCM-22>HM. The performance of the zeolites has been largely improved after the modification. Naphthalene conversion rate reaches 97% and 60%, andβ,β′-selectivity 66% and 70% for CuHY and CuH?, respectively. Metal surfactants, such as hexanoic and octanoic copper, play a positive role in modifying the external surface and pore structure of zeolitesβ and Y. 129Xe NMR results demonstrate that the two types of the pore channels in CuHβ are unimpeded for xenon atoms, and there is a fast chemical exchange between two xenon atoms located in different adsorption sites; Cu2+ ion is a strong adsorption site for xenon atoms and it is a strong active center as well; Cu2+ and Cu+ ions coexist in channels of zeolites, which are in agreement with the conclusions from ab initio quantum chemical calculations.

  14. Conversion of the bifunctional 8-oxoguanine/beta-delta apurinic/apyrimidinic DNA repair activities of Drosophila ribosomal protein S3 into the human S3 monofunctional beta-elimination catalyst through a single amino acid change.

    Science.gov (United States)

    Hegde, V; Kelley, M R; Xu, Y; Mian, I S; Deutsch, W A

    2001-07-20

    The Drosophila S3 ribosomal protein has important roles in both protein translation and DNA repair. In regards to the latter activity, it has been shown that S3 contains vigorous N-glycosylase activity for the removal of 8-oxoguanine residues in DNA that leaves baseless sites in their places. Drosophila S3 also possesses an apurinic/apyrimidinic (AP) lyase activity in which the enzyme catalyzes a beta-elimination reaction that cleaves phosphodiester bonds 3' and adjacent to an AP lesion in DNA. In certain situations, this is followed by a delta-elimination reaction that ultimately leads to the formation of a single nucleotide gap in DNA bordered by 5'- and 3'-phosphate groups. The human S3 protein, although 80% identical to its Drosophila homolog and shorter by only two amino acids, has only marginal N-glycosylase activity. Its lyase activity only cleaves AP DNA by a beta-elimination reaction, thus further distinguishing itself from the Drosophila S3 protein in lacking a delta-elimination activity. Using a hidden Markov model analysis based on the crystal structures of several DNA repair proteins, the enzymatic differences between Drosophila and human S3 were suggested by the absence of a conserved glutamine residue in human S3 that usually resides at the cleft of the deduced active site pocket of DNA glycosylases. Here we show that the replacement of the Drosophila glutamine by an alanine residue leads to the complete loss of glycosylase activity. Unexpectedly, the delta-elimination reaction at AP sites was also abrogated by a change in the Drosophila glutamine residue. Thus, a single amino acid change converted the Drosophila activity into one that is similar to that possessed by the human S3 protein. In support of this were experiments executed in vivo that showed that human S3 and the Drosophila site-directed glutamine-changed S3 performed poorly when compared with Drosophila wild-type S3 and its ability to protect a bacterial mutant from the harmful effects of

  15. Influence of Steam Treating on Deethylating Type Isomerization Catalyst

    Institute of Scientific and Technical Information of China (English)

    2005-01-01

    This article mainly worked on methods to reduce side reactions of the de-ethylating type catalyst for xylene isomerization. In laboratory the de-ethylating type catalyst for xylene isomerization was subjected to steam treatment at different temperatures and durations to achieve dealumination of the ZSM-5 zeolite to some extent, which could affect the change in Bronsted acid content to decrease xylene loss along with reduction of side reactions. Test results showed that the degree for reducing side reactions by steam treatment depended upon two important parameters-treating temperature and duration. The optimal condition required treating the catalyst at 500℃ for 8 hours.

  16. INVESTIGATION ON Pd/Beta CATALYST IN HEXANE ISOMERIZATION%正己烷异构化Pd/Seta催化剂的研究

    Institute of Scientific and Technical Information of China (English)

    李旭; 王昕; 施力; 韩松

    2004-01-01

    通过临氢微型反应器,在反应压力2 MPa、温度260℃、质量空速2 h-1、氢油摩尔比4:1的条件下,以正己烷为原料对钯质量分数为0.1%,0.2%,0.3%,0.4%,0.5%的五种Pd/Beta 催化剂进行了评价,其裂解率分别为2.79%,2.00%,1.13%,0.63%,0.53%,裂解率随着钯质量分数的增加而减少;在考察的范围内,催化剂的活性、选择性、异构化率均随着钯质量分数的增加而上升,钯质量分数为0.3%时,选择性最好为17.94%,钯质量分数大于0.2%时,转化率和异构化率趋于稳定,转化率为82%左右,异构化率为80%左右.

  17. Metal immobilization in soils using synthetic zeolites.

    Science.gov (United States)

    Oste, Leonard A; Lexmond, Theo M; Van Riemsdijk, Willem H

    2002-01-01

    In situ immobilization of heavy metals in contaminated soils is a technique to improve soil quality. Synthetic zeolites are potentially useful additives to bind heavy metals. This study selected the most effective zeolite in cadmium and zinc binding out of six synthetic zeolites (mordenite-type, faujasite-type, zeolite X, zeolite P, and two zeolites A) and one natural zeolite (clinoptilolite). Zeolite A appeared to have the highest binding capacity between pH 5 and 6.5 and was stable above pH 5.5. The second objective of this study was to investigate the effects of zeolite addition on the dissolved organic matter (DOM) concentration. Since zeolites increase soil pH and bind Ca, their application might lead to dispersion of organic matter. In a batch experiment, the DOM concentration increased by a factor of 5 when the pH increased from 6 to 8 as a result of zeolite A addition. A strong increase in DOM was also found in the leachate of soil columns, particularly in the beginning of the experiment. This resulted in higher metal leaching caused by metal-DOM complexes. In contrast, the free ionic concentration of Cd and Zn strongly decreased after the addition of zeolites, which might explain the reduction in metal uptake observed in plant growth experiments. Pretreatment of zeolites with acid (to prevent a pH increase) or Ca (to coagulate organic matter) suppressed the dispersion of organic matter, but also decreased the metal binding capacity of the zeolites due to competition of protons or Ca.

  18. New Trends in Gold Catalysts

    Directory of Open Access Journals (Sweden)

    Leonarda F. Liotta

    2014-07-01

    Full Text Available Gold is an element that has fascinated mankind for millennia. The catalytic properties of gold have been a source of debate, due to its complete chemical inertness when in a bulk form, while it can oxidize CO at temperatures as low as ~200 K when in a nanocrystalline state, as discovered by Haruta in the late 1980s [1]. Since then, extensive activity in both applied and fundamental research on gold has been initiated. The importance of the catalysis by gold represents one of the fasted growing fields in science and is proven by the promising applications in several fields, such as green chemistry and environmental catalysis, in the synthesis of single-walled carbon nanotubes, as modifiers of Ni catalysts for methane steam and dry reforming reactions and in biological and electrochemistry applications. The range of reactions catalyzed by gold, as well as the suitability of different supports and the influence of the preparation conditions have been widely explored and optimized in applied research [2]. Gold catalysts appeared to be very different from the other noble metal-based catalysts, due to their marked dependence on the preparation method, which is crucial for the genesis of the catalytic activity. Several methods, including deposition-precipitation, chemical vapor deposition and cation adsorption, have been applied for the preparation of gold catalysts over reducible oxides, like TiO2. Among these methods, deposition-precipitation has been the most frequently employed method for Au loading, and it involves the use of tetrachloroauric (III acid as a precursor. On the other hand, the number of articles dealing with Au-loaded acidic supports is smaller than that on basic supports, possibly because the deposition of [AuCl4]− or [AuOHxCl4−x]− species on acidic supports is difficult, due to their very low point of zero charge. Despite this challenge, several groups have reported the use of acidic zeolites as supports for gold. Zeolites

  19. Catalytic activity in individual cracking catalyst particles imaged throughout different life stages by selective staining

    Science.gov (United States)

    Buurmans, Inge L. C.; Ruiz-Martínez, Javier; Knowles, William V.; van der Beek, David; Bergwerff, Jaap A.; Vogt, Eelco T. C.; Weckhuysen, Bert M.

    2011-11-01

    Fluid catalytic cracking (FCC) is the major conversion process used in oil refineries to produce valuable hydrocarbons from crude oil fractions. Because the demand for oil-based products is ever increasing, research has been ongoing to improve the performance of FCC catalyst particles, which are complex mixtures of zeolite and binder materials. Unfortunately, there is limited insight into the distribution and activity of individual zeolitic domains at different life stages. Here we introduce a staining method to visualize the structure of zeolite particulates and other FCC components. Brønsted acidity maps have been constructed at the single particle level from fluorescence microscopy images. By applying a statistical methodology to a series of catalysts deactivated via industrial protocols, a correlation is established between Brønsted acidity and cracking activity. The generally applicable method has clear potential for catalyst diagnostics, as it determines intra- and interparticle Brønsted acidity distributions for industrial FCC materials.

  20. NO.sub.x catalyst and method of suppressing sulfate formation in an exhaust purification system

    Science.gov (United States)

    Balmer-Millar, Mari Lou; Park, Paul W.; Panov, Alexander G.

    2007-06-26

    The activity and durability of a zeolite lean-burn NOx catalyst can be increased by loading metal cations on the outer surface of the zeolite. However, the metal loadings can also oxidize sulfur dioxide to cause sulfate formation in the exhaust. The present invention is a method of suppressing sulfate formation in an exhaust purification system including a NO.sub.x catalyst. The NO.sub.x catalyst includes a zeolite loaded with at least one metal. The metal is selected from among an alkali metal, an alkaline earth metal, a lanthanide metal, a noble metal, and a transition metal. In order to suppress sulfate formation, at least a portion of the loaded metal is complexed with at least one of sulfate, phosphate, and carbonate.