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The Crystal Cavities of the New Jersey Zeolite Region

Description: From abstract: The crystal cavities present in the mineral complex of the New Jersey traprock region have long excited the interest of mineralogists. In 1914 Fenner made the first detailed and comprehensive study of these cavities and suggested that babingtonite was the original mineral. Soon after this anhydrite was found occupying parts of some of the cavities at one of the quarries. At this time, too, Wherry concluded that glauberite was the original mineral of some of the cavities because of his studies of similar crystal cavities in Triassic shale at different places.
Date: 1932
Creator: Schaller, Waldemar T.
Partner: UNT Libraries Government Documents Department

Molecular Dynamics Simulations of Hexadecane/Silicalite Interfaces

Description: The interface between liquid hexadecane and the (010) surface of silicalite was studied by molecular dynamics. The structure of molecules in the interracial region is influenced by the presence of pore mouths on the silicalite surface. For this surface, whose pores are the entrances to straight channels, the concentration profile for partially absorbed molecules is peaked around 10 monomers inside the zeolite. No preference to enter or exit the zeolite based on absorption length is observed except for very small or very large absorption lengths. We also found no preferential conformation of the unabsorbed tails for partially absorbed molecules.
Date: January 20, 1999
Creator: Grest, G.S. & Webb, E.B.
Partner: UNT Libraries Government Documents Department

"A Novel Synthesis of Zeolite W..."

Description: Zeolite W has been synthesized using organometallic silicon and aluminum precursors in two hydrothermal systems: organocation containing and organocation-free. The reaction using the organocation yielded a fully crystalline, relatively uniform crystal size product, with no organic molecules occluded in the pores. In contrast, the product obtained from an identical reaction, except for the absence of the organocation, contained amorphous as well as crystalline material and the crystalline phase showed a large diversity of both crystal size and morphology. The use of organometallic precursors, either with or without an organocation, allows for the crystallization of the MER framework at much lower 0H/Si02 and (K+ Na - Al)/Si ratios than is typical of inorganic systems. The reaction products were characterized by XRD, SEM, EDS, and thermal analyses.
Date: May 7, 1999
Creator: Nenoff, Tina M. & Thoma, Steven G.
Partner: UNT Libraries Government Documents Department

Photochemical charge separation in zeolites: Electron transfer dynamics, nanocrystals and zeolitic membranes. Final technical report

Description: Aluminosilicate zeolites provide an excellent host for photochemical charge separation. Because of the constraints provided by the zeolite, the back electron transfer from the reduced acceptor to the oxidized sensitizer is slowed down. This provides the opportunity to separate the charge and use it in a subsequent reaction for water oxidation and reduction. Zeolite-based ruthenium oxide catalysts have been found to be efficient for the water splitting process. This project has demonstrated the usefulness of zeolite hosts for photolytic splitting of water.
Date: September 30, 2001
Creator: Dutta, Prabir K.
Partner: UNT Libraries Government Documents Department

An experimental and density functional theory study of the interactions of CH4 with H-ZSM-5

Description: The interactions of methane with Bronsted acid sites in H-ZSM-5 were investigated both experimentally and theoretically. Diffuse reflectance infrared spectroscopy was used to acquire spectra for methane adsorbed on H-ZSM-5 at room temperature and at 77 K. Upon adsorption, the v1 and v3 vibrational bands of methane shift by -15 and -23 cm-1, respectively, and the vibrational band for OH groups associated with Bronsted acid sites shifts by -93 cm-1. Quantum chemical calculations conducted at the DFT level of theory with a 6-31g**++ basis set show that the observed shifts for methane are attributable to the effects of the electrostatic field created by the atoms of the zeolite. To represent the influence of the zeolite on the adsorbed methane correctly, it is essential to take into account the effects of the Madelung field, as well as the local effects of the acid center. The calculated shift in the vibrational frequency of the bridging OH group lies within the range observed experimentally. However, the quantitative agreement of the calculated and observed shift is not as good as that seen for the bands of CH4.
Date: August 25, 2001
Creator: Khaliullin, Rustam Z.; Bell, Alexis T. & Kazansky, Vladimir B.
Partner: UNT Libraries Government Documents Department

Zeolite thermodynamics and kinetics. Final report for June 15, 1996 to June 15, 2000 to the U.S. Department of Energy, Geosciences Research Program, Office of Basic Energy Sciences on Grant No. DE-FG02-96ER14634

Description: This report summarizes results obtained on the thermodynamic and kinetic properties of zeolites. DOE funding supported the development of techniques of material preparation as well as experimental strategies and methods for measuring solubilities, hydration states, and rates of zeolite dissolution, precipitation, and nucleation. The hydrothermal experiments provided temperature-dependent solubility products, hydration states, and a set of standard free energies of formation for end-member Na-, K-, and Ca-clinoptilolite, mordenite, and analcime. Flow-through experimental methods were used to measure the rates of Na-clinoptilolite and analcime dissolution and precipitation as a function of reaction affinity to 250C. Finally, the experimental system was modified so that the clinoptilolite-to-analcime transformation was monitored, and its rates and mechanisms were evaluated.
Date: June 15, 2000
Creator: Barnes, H. L.; Wilkin, R. T. & Benning, L. G.
Partner: UNT Libraries Government Documents Department

Treatment of Produced Water Using a Surfactant Modified Zeolite/Vapor Phase Bioreactor System

Description: Co-produced water from the oil and gas industry accounts for a significant waste stream in the United States. Produced waters typically contain a high total dissolved solids content, dissolved organic constituents such as benzene and toluene, an oil and grease component as well as chemicals added during the oil-production process. It has been estimated that a total of 14 billion barrels of produced water were generated in 2002 from onshore operations (Veil, 2004). Although much of this produced water is disposed via reinjection, environmental and cost considerations can make surface discharge of this water a more practical means of disposal. In addition, reinjection is not always a feasible option because of geographic, economic, or regulatory considerations. In these situations, it may be desirable, and often necessary from a regulatory viewpoint, to treat produced water before discharge. It may also be feasible to treat waters that slightly exceed regulatory limits for re-use in arid or drought-prone areas, rather than losing them to reinjection. A previous project conducted under DOE Contract DE-AC26-99BC15221 demonstrated that surfactant modified zeolite (SMZ) represents a potential treatment technology for produced water containing BTEX. Laboratory and field experiments suggest that: (1) sorption of benzene, toluene, ethylbenzene and xylenes (BTEX) to SMZ follows linear isotherms in which sorption increases with increasing solute hydrophobicity; (2) the presence of high salt concentrations substantially increases the capacity of the SMZ for BTEX; (3) competitive sorption among the BTEX compounds is negligible; and, (4) complete recovery of the SMZ sorption capacity for BTEX can be achieved by air sparging the SMZ. This report summarizes research for a follow on project to optimize the regeneration process for multiple sorption/regeneration cycles, and to develop and incorporate a vapor phase bioreactor (VPB) system for treatment of the off-gas generated during air sparging. To this end, we ...
Date: January 31, 2006
Creator: Katz, Lynn E.; Kinney, Kerry A.; Bowman, Robert S.; Sullivan, Enid J.; Kwon, Soondong; Darby, Elaine B. et al.
Partner: UNT Libraries Government Documents Department

Treatment of Produced Waters Using a Surfactant Modified Zeolite/Vapor Phase Bioreactor System

Description: This report summarizes work performed on this project from April 2004 through September 2004. Our previous work demonstrated that a polyurethane foam biofilter could successfully biodegrade the BTEX contaminants found in the SMZ regeneration waste gas stream. However, establishing the biomass on the polyurethane foam packing was relatively time consuming and daily recirculation of a concentrated nutrient solution was required for efficient operation of the foam biofilter. To simplify the start up and operating requirements of the biofilter system, a simple, compost-based biofilter was investigated for its ability to treat the BTEX contaminants generated during the SMZ regeneration process. The investigation of the compost biofilter was divided into three experimental phases that spanned 180 days of biofilter operation. During Phase 1, the biofilter was continuously supplied a BTEX-contaminated waste gas stream. During Phase 2, a series of periodic shutdown tests were conducted to assess how the biofilter responded when the BTEX feed was discontinued for periods ranging from 1 day to 2.8 days. The Phase 3 experiments focused on determining how the biofilter would handle periodic spikes in inlet BTEX concentration as would be expected when it is coupled with an SMZ column. Results from the continuous feed (Phase 1) experiments demonstrated that the compost biofilter could maintain BTEX removals of greater than 98% within two weeks of startup. Results of the shutdown experiments indicated that benzene removal was the most sensitive to interruptions in the BTEX feed. Nevertheless, the BTEX removal efficiency exceeded 95% within 6 hours of reestablishing the BTEX feed to the biofilter. When the biofilter was subjected to periodic spikes in BTEX concentration (Phase 3), it was found that the total BTEX removal efficiency stabilized at approximately 75% despite the fact that the biofilter was only fed BTEX contaminants 8 hours per day. Finally, the effects ...
Date: September 11, 2004
Creator: Katz, Lynn E.; Kinney, Kerry A.; Bowman, R. S. & Sullivan, E. J.
Partner: UNT Libraries Government Documents Department

Suspending Zeolite Particles In Tanks

Description: The Savannah River Site (SRS) is in the process of removing waste (sludge and salt cake) from million gallon waste tanks. The current practice for removing waste from the tanks is adding water, agitating the tanks with long shaft vertical centrifugal pumps, and pumping the sludge/salt solution from the tank to downstream treatment processes. This practice has left sludge heels ({tilde} 30,000 gallons) in the bottom of the tanks. SRS is evaluating shrouded axial impeller mixers for removing the sludge heels in the waste tanks. The authors conducted a test program to determine mixer requirements for suspending sludge heels using the shrouded axial impeller mixers. The tests were performed with zeolite in scaled tanks which have diameters of 1.5, 6.0, and 18.75 feet. The mixer speeds required to suspend zeolite particles were measured at each scale. The data were analyzed with various scaling methods to compare their ability to describe the suspension of insoluble solids with the mixers and to apply the data to a full-scale waste tank. The impact of changes in particle properties and operating parameters was also evaluated. The conclusions of the work are: Scaling of the suspension of fast settling zeolite particles was best described by the constant power per unit volume method. Increasing the zeolite particle concentration increased the required mixer power needed to suspend the particles. Decreasing the zeolite particle size from 0.7 mm � 0.3 mm decreased the required mixer power needed to suspend the particles. Increasing the number of mixers in the tank decreased the required mixer power needed to suspend the particles. A velocity of 1.6 ft/sec two inches above the tank bottom is needed to suspend zeolite particles.
Date: January 19, 1999
Creator: Poirier, M.R.
Partner: UNT Libraries Government Documents Department

Thermodynamic modeling of natural zeolite stability

Description: Zeolites occur in a variety of geologic environments and are used in numerous agricultural, commercial, and environmental applications. It is desirable to understand their stability both to predict future stability and to evaluate the geochemical conditions resulting in their formation. The use of estimated thermodynamic data for measured zeolite compositions allows thermodynamic modeling of stability relationships among zeolites in different geologic environments (diagenetic, saline and alkaline lakes, acid rock hydrothermal, basic rock, deep sea sediments). This modeling shows that the relative cation abundances in both the aqueous and solid phases, the aqueous silica activity, and temperature are important factors in determining the stable zeolite species. Siliceous zeolites (e.g., clinoptilolite, mordenite, erionite) present in saline and alkaline lakes or diagenetic deposits formed at elevated silica activities. Aluminous zeolites (e.g., natrolite, mesolite/scolecite, thomsonite) formed in basic rocks in association with reduced silica activities. Likewise, phillipsite formation is favored by reduced aqueous silica activities. The presence of erionite, chabazite, and phillipsite are indicative of environments with elevated potassium concentrations. Elevated temperature, calcic water conditions, and reduced silica activity help to enhance the laumontite and wairakite stability fields. Analcime stability increases with increased temperature and aqueous Na concentration, and/or with decreased silica activity.
Date: June 1, 1997
Creator: Chipera, S. J. & Bish, D. L.
Partner: UNT Libraries Government Documents Department

Vapor Phase Transport Synthesis of Zeolites from Sol-Gel Precursors

Description: A study of zeolite crystallization from sol-gel precursors using the vapor phase transport synthesis method has been performed. Zeolites (ZSM-5, ZSM-48, Zeolite P, and Sodalite) were crystallized by contacting vapor phase organic or organic-water mixtures with dried sodium silicate and dried sodium alumino-silicate gels. For each precursor gel, a ternary phase system of vapor phase organic reactant molecules was explored. The vapor phase reactant mixtures ranged from pure ethylene diamene, triethylamine, or water, to an equimolar mixture of each. In addition, a series of gels with varied physical and chemical properties were crystallized using the same vapor phase solvent mixture for each gel. The precursor gels and the crystalline products were analyzed via Scanning Electron Microscopy, Electron Dispersive Spectroscopy, X-ray mapping, X-ray powder diffraction, nitrogen surface area, Fourier Transform Infrared Spectroscopy, and thermal analyses. The product phase and purity as a function of the solvent mixture, precursor gel structure, and precursor gel chemistry is discussed.
Date: July 14, 2000
Partner: UNT Libraries Government Documents Department

Co-adsorption studies of hydrogen with nitrogen in zeolites

Description: The use of co-adsorption studies of N{sub 2} with H{sub 2} makes it possible to obtain information about adsorption of N{sub 2} by monitoring changes in the rotational spectrum of the co-adsorbed H{sub 2} molecules. The authors present such results on N{sub 2}/H{sub 2} in Na-13X. The authors have demonstrated that inelastic neutron scattering studies of H{sub 2} co-adsorbed with other molecules can be used as an effective probe of their adsorption sites and interactions with zeolite hosts. Simulation studies are clearly required for extracting the wealth of detail which is evident in these data.
Date: August 1998
Creator: Eckert, J.; Trouw, F. R. & McMenomy, M.
Partner: UNT Libraries Government Documents Department

Multitechnique Analysis of the Lattice Structures of Highly Siliceous Zeolites

Description: The combined use of high-resolution solid state NMR techniques (both 1D and 2D) with synchrotron-based powder x-ray diffraction studies yields detailed information on the lattice structures of highly siliceous zeolites. The two methods are complementary, the former probing short range ordering and structures while the latter is sensitive to long range orderings and periodicities.
Date: August 26, 1999
Creator: Fyfe, C. A.; Gies, H.; Kokotailo, G. T.; Feng, Y.; Strobl, H.; Marler, B. et al.
Partner: UNT Libraries Government Documents Department


Description: Selective occlusions of straight-chain paraffins in the presence of branched-chain hydrocarbons by naturally occurring zeolites of suitable dimension was reported as early as 1944 by Barrer and Ibbitson. More recently the capacity of synthetic zeolites or molecular sieves to absorb exclusively the straight-chain hydrocarbons from complex hydrocarbon mixtures has found extensive application in the petroleum industry. Under the conditions developed for most sieving operations any normal olefins present are occluded along with the normal paraffins. A supplemental separation technique must be employed to obtain n-paraffins free of olefins.
Date: August 30, 1966
Creator: Fenselau, Catherine & Calvin, Melvin
Partner: UNT Libraries Government Documents Department

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

Description: 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.
Date: March 31, 2007
Creator: Ingram, Conrad & Mitchell, Mark
Partner: UNT Libraries Government Documents Department

Treatment of Produced Waters Using a Surfactant Modified Zeolite/Vapor Phase Bioreactor System

Description: This report summarizes work of this project from October 2003 through March 2004. The major focus of the research was to further investigate BTEX removal from produced water, to quantify metal ion removal from produced water, and to evaluate a lab-scale vapor phase bioreactor (VPB) for BTEX destruction in off-gases produced during SMZ regeneration. Batch equilibrium sorption studies were conducted to evaluate the effect of semi-volatile organic compounds commonly found in produced water on the sorption of benzene, toluene, ethylbenzene, and xylene (BTEX) onto surfactant-modified zeolite (SMZ) and to examine selected metal ion sorption onto SMZ. The sorption of polar semi-volatile organic compounds and metals commonly found in produced water onto SMZ was also investigated. Batch experiments were performed in a synthetic saline solution that mimicked water from a produced water collection facility in Wyoming. Results indicated that increasing concentrations of semi-volatile organic compounds increased BTEX sorption. The sorption of phenol compounds could be described by linear isotherms, but the linear partitioning coefficients decreased with increasing pH, especially above the pKa's of the compounds. Linear correlations relating partitioning coefficients of phenol compounds with their respective solubilities and octanol-water partitioning coefficients were developed for data collected at pH 7.2. The sorption of chromate, selenate, and barium in synthetic produced water were also described by Langmuir isotherms. Experiments conducted with a lab-scale vapor phase bioreactor (VPB) packed with foam indicated that this system could achieve high BTEX removal efficiencies once the nutrient delivery system was optimized. The xylene isomers and benzene were found to require the greatest biofilter bed depth for removal. This result suggested that these VOCs would ultimately control the size of the biofilter required for the produced water application. The biofilter recovered rapidly from shutdowns showing that the system was resilient to discontinuous feed conditions therefore provided flexibility on ...
Date: March 11, 2004
Creator: Katz, Lynn E.; Kinney, Kerry A.; Bowman, R. S. & Sullivan, E. J.
Partner: UNT Libraries Government Documents Department

Treatment of Produced Waters Using a Surfactant Modified Zeolite/Vapor Phase Bioreactor System

Description: This report summarizes work performed on this project from October 2004 through March 2005. In previous work, a surfactant modified zeolite (SMZ) was shown to be an effective system for removing BTEX contaminants from produced water. Additional work on this project demonstrated that a compost-based biofilter could biodegrade the BTEX contaminants found in the SMZ regeneration waste gas stream. However, it was also determined that the BTEX concentrations in the waste gas stream varied significantly during the regeneration period and the initial BTEX concentrations were too high for the biofilter to handle effectively. A series of experiments were conducted to determine the feasibility of using a passive adsorption column placed upstream of the biofilter to attenuate the peak gas-phase VOC concentrations delivered to the biofilter during the SMZ regeneration process. In preparation for the field test of the SMZ/VPB treatment system in New Mexico, a pilot-scale SMZ system was also designed and constructed during this reporting period. Finally, a cost and feasibility analysis was also completed. To investigate the merits of the passive buffering system during SMZ regeneration, two adsorbents, SMZ and granular activated carbon (GAC) were investigated in flow-through laboratory-scale columns to determine their capacity to handle steady and unsteady VOC feed conditions. When subjected to a toluene-contaminated air stream, the column containing SMZ reduced the peak inlet 1000 ppmv toluene concentration to 630 ppmv at a 10 second contact time. This level of buffering was insufficient to ensure complete removal in the downstream biofilter and the contact time was longer than desired. For this reason, using SMZ as a passive buffering system for the gas phase contaminants was not pursued further. In contrast to the SMZ results, GAC was found to be an effective adsorbent to handle the peak contaminant concentrations that occur early during the SMZ regeneration ...
Date: March 11, 2005
Creator: Kwon, Soondong; Darby, Elaine B.; Chen, Li-Jung; Katz, Lynn E.; Kinney, Kerry A.; Bowman, R. S. et al.
Partner: UNT Libraries Government Documents Department

Effect of different glass and zeolite A compositions on the leach resistance of ceramic waste forms

Description: A ceramic waste form is being developed for waste generated during electrometallurgical treatment of spent nuclear fuel. The waste is generated when fission products are removed from the electrolyte, LiCl-KCl eutectic. The waste form is a composite fabricated by hot isostatic pressing a mixture of glass frit and zeolite occluded with fission products and salt. Normalized release rate is less than 1 g/m{sup 2}d for all elements in MCC-1 leach test run for 28 days in deionized water at 90 C. This leach resistance is comparable to that of early Savannah River glasses. We are investigating how leach resistance is affected by changes in cationic form of zeolite and in glass composition. Composites were made with 3 forms of zeolite A and 6 glasses. We used 3-day ASTM C1220-92 (formerly MCC-1) leach tests to screen samples for development purposes only. The leach test results show that the glass composites of zeolites 5A and 4A retain fission products equally well. Loss of Cs is small (0.1-0.5 wt%), while the loss of divalent and trivalent fission products is one or more orders of magnitude smaller. Composites of 5A retain chloride ion better in these short-term screens than 4A and 3A. The more leach resistant composites were made with durable glasses rich in silica and poor in alkaline earth oxides. XRD show that a salt phase was absent in the leach resistant composites of 5A and the better glasses but was present in the other composites with poorer leach performance. Thus, absence of salt phase corresponds to improved leach resistance. Interactions between zeolite and glass depend on composition of both.
Date: December 1996
Creator: Lewis, M. A.; Hash, M. & Glandorf, D.
Partner: UNT Libraries Government Documents Department

Effect of different glasses in glass bonded zeolite

Description: A mineral waste form has been developed for chloride waste salt generated during the pyrochemical treatment of spent nuclear fuel. The waste form consists of salt-occluded zeolite powders bound within a glass matrix. The zeolite contains the salt and immobilizes the fission products. The zeolite powders are hot pressed to form a mechanically stable, durable glass bonded zeolite. Further development of glass bonded zeolite as a waste form requires an understanding of the interaction between the glass and the zeolite. Properties of the glass that enhance binding and durability of the glass bonded zeolite need to be identified. Three types of glass, boroaluminosilicate, soda-lime silicate, and high silica glasses, have a range of properties and are now being investigated. Each glass was hot pressed by itself and with an equal amount of zeolite. MCC-1 leach tests were run on both. Soda-lime silicate and high silica glasses did not give a durable glass bonded zeolite. Boroaluminosilicate glasses rich in alkaline earths did bind the zeolite and gave a durable glass bonded zeolite. Scanning electron micrographs suggest that the boroaluminosilicate glasses wetted the zeolite powders better than the other glasses. Development of the glass bonded zeolite as a waste form for chloride waste salt is continuing.
Date: May 1, 1995
Creator: Lewis, M.A.; Ackerman, J.P. & Verma, S.
Partner: UNT Libraries Government Documents Department

Pulsed laser deposition of zeolitic membranes

Description: The pulsed laser deposition of zeolites to form zeolitic thin films is described. Films were grown using both mordenite and faujasite targets and were deposited on various substrates. The optimal films were obtained when the target and substrate were separated by 5 cm. These films are comprised of small crystallites embedded in an amorphous matrix. Transmission electron microscopy reveals that the amorphous material is largely porous and that the pores appear to be close to the same size as the parent zeolite. Zeolotic thin films are of interest for sensor, gas separation, and catalytic applications.
Date: February 1, 1995
Creator: Peachey, N.M.; Dye, R.C. & Ries, P.D.
Partner: UNT Libraries Government Documents Department