FAU-Type Zeolite Synthesis from Clays and Its Use for the Simultaneous Adsorption of Five Divalent Metals from Aqueous Solutions.
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ABSTRACT:
SUBMITTER: Joseph IV
PROVIDER: S-EPMC8269868 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Natural clay particles have been hypothesized as catalysts on the early Earth, potentially facilitating the formation of early organic (bio) molecules. Association of clay particles with droplets formed by liquid-liquid phase separation could provide a physical mechanism for compartmentalization of inorganic catalysts in primitive protocells. Here we explore the distribution of natural clay mineral particles in poly(ethylene glycol) (PEG)/dextran (Dx) aqueous two-phase systems (ATPS). We compared the three main types of natural clay: kaolinite, montmorillonite and illite, all of which are aluminosilicates of similar composition and surface charge. The three clay types differ in particle size, crystal structure, and their accumulation at the ATPS interface and ability to stabilize droplets against coalescence. Illite and kaolinite accumulated at the aqueous/aqueous interface, stabilizing droplets against coalescence but not preventing their eventual sedimentation due to the mass of adsorbed particles. The ability of each clay-containing ATPS to catalyze reaction of o-phenylenediamine with peroxide to form 2,3-diaminophenazone was evaluated. We observed modest rate increases for this reaction in the presence of clay-containing ATPS over clay in buffer alone, with illite outperforming the other clays. These findings are encouraging because they support the potential of combining catalytic mineral particles with aqueous microcompartments to form primitive microreactors.
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Project description:In order to realize designed synthesis, understanding the formation mechanism of zeolites at an atomic level has long been aspired, but remains challenging due to the fact that the knowledge of atomic configurations of the species formed during the process is limited. We focus on a synthesis system that crystallizes CHA zeolite from FAU zeolite as the sole source of tetrahedral atoms of Si and Al, so that end-to-end characterization can be conducted. Solid-state 29Si MAS NMR is followed by high-throughput computational modeling to understand how atomic configurations changed during the interzeolite conversion. This reveals that the structural motif commonly found in FAU and CHA is not preserved during the conversion; rather, there is a specific rearrangement of silicates and aluminates within the motif. The atomic configuration of CHA seems to be influenced by that of the starting FAU, considering that CHA synthesized without using FAU results in a random Al distribution. A Metropolis Monte-Carlo simulation combined with a lattice minimization technique reveals that CHA derived from FAU has energetically favorable, biased atomic locations, which could be a result of the atomic configurations of the starting FAU. These results suggest that by choosing the appropriate reactant, Al placement could be designed to enhance the targeted properties of zeolites for catalysis and adsorption.
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Project description:Zeolite-geopolymer hybrid materials have been formed when kaolin was used as a starting material. Their characteristics are of interest because they can have a wide pore size distribution with micro- and meso-pores due to the zeolite and geopolymer, respectively. In this study, Zeolite-geopolymer hybrid bulk materials were fabricated using four kinds of kaolinitic clays (a halloysite and three kinds of kaolinite). The kaolinitic clays were first calcined at 700 °C for 3 h to transform into the amorphous aluminosilicate phases. Alkali-activation treatment of the metakaolin yielded bulk materials with different amounts and types of zeolite and different compressive strength. This study investigated the effects of the initial kaolinitic clays on the amount and types of zeolite in the resultant geopolymers as well as the strength of the bulk materials. The kaolinitic clays and their metakaolin were characterized by XRD analysis, chemical composition, crystallite size, 29Si and 27Al MAS NMR analysis, and specific surface area measurements. The correlation between the amount of zeolite formed and the compressive strength of the resultant hybrid bulk materials, previously reported by other researchers was not positively observed. In the studied systems, the effects of Si/Al and crystalline size were observed. When the atomic ratio of Si/Al in the starting kaolinitic clays increased, the compressive strength of the hybrid bulk materials increased. The crystallite size of the zeolite in the hybrid bulk materials increased with decreasing compressive strength of the hybrid bulk materials.
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Project description:The preparation of metastable zeolites is often restricted to a limited range of synthesis conditions, which is exemplified in commercial syntheses lacking organics to stabilize the crystal structure. In the absence of an organic structure-directing agent, interzeolite transformation is a common phenomenon that can lead to undesirable products or impurities. Many studies have investigated the substitution of Si and Al in zeolite frameworks with alternative elements (heteroatoms) as a means of tailoring the properties of zeolites; however, relatively few studies have systematically explored the impact of heteroatoms on interzeolite transformations and their concomitant effects on zeolite crystallization. In this study, we examine methods to prepare isostructures of faujasite (FAU), which is one of the most commercially relevant zeolites and also a thermodynamically metastable structure. A survey of multivalent elements revealed that zinc is capable of stabilizing FAU at high temperatures and inhibiting its frequent transformation to zeolite gismondine (GIS). Using combined experimental and computational studies, we show that zinc alters the chemical nature of growth mixtures by sequestering silicates. Zinc heteroatoms incorporate in the FAU framework with a loading-dependent coordination. Our collective findings provide an improved understanding of driving forces for the FAU-to-GIS interzeolite transformation where we observe that heteroatoms (e.g., zinc) can stabilize zeolite FAU over a broad range of synthesis conditions. Given the growing interest in heteroatom-substituted zeolites, this approach to preparing zinc-containing FAU may prove applicable to a broader range of zeolite structures.
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Project description:Silicone and pure organic binders were used to develop FAU-type zeolite coatings applied on pre-treated aluminum substrates by using a spraying method and then cured under specific conditions. The influence of the amount of binder on adhesion properties of zeolite coatings was first investigated to determine the optimum ratio between zeolite and binder. Zeolite coatings were then elaborated with a high zeolite content (between 70 and 80 wt.%) to ensure high adsorption capacities. The amount of binders involved in different zeolite coatings was sufficient to achieve interesting adhesion and cohesion properties. The accessibility of zeolite microporosity was studied by nitrogen adsorption-desorption measurements, which revealed a very small or no loss of the micropore volume for the optimized coatings. Volatile Organic Compounds (VOCs) adsorption measurements were carried out using n-hexane as probe molecule. FAU-type zeolite in powder form adsorbs 180 mg/ganhydrous zeolite, whereas the amounts of n-hexane adsorbed by zeolite coatings ranged from 131 to 175 mg/ganhydrous zeolite.
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Project description:The highly efficient removal of tetracycline (TC) from an aqueous solution was accomplished by using the raw shrimp shell waste (SSW) as an environmentally friendly adsorbent. The SSW without any treatment removed TC more efficiently than the SSW after being treated with HCl and NaOH solutions. The SSW was characterized using nitrogen adsorption-desorption isotherms, scanning electron microscopy alongside energy-dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, a thermogravimetric-derivative thermogravimetry analyzer, and a ?-potential analyzer. The maximum adsorption capacity of 400 mg/L SSW was 229.98 mg/g for 36 h at 55 °C. Both the Langmuir isotherm model and the pseudo-second-order kinetic model well described the experimental data. According to the values of the Gibbs free energy and enthalpy changes, the TC adsorption by SSW proved to be spontaneous and endothermic. The TC adsorption process was controlled by intraparticle diffusion and liquid film diffusion.
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Project description:The adsorption behavior of Cr(III) and Cr(VI) ions onto laboratory-synthesized 2-line ferrihydrite was investigated under a batch method as a function of initial chromium concentration (0.1-1000 mg L-1) and pH (3.0 and 5.0). Moreover, the effect of the type of anion (chloride and sulfate) on Cr(III) adsorption was studied. The affinity of Cr(III) ions for the ferrihydrite surface depended on both the type of anion and pH of the solution and the maximum adsorption capacities decreased as follows: q (SO4 2-, pH 5.0) > q (SO4 2-, pH 3.0) > q (Cl-, pH 5.0) > q (Cl-, pH 3.0), and were found to be 86.06 mg g-1, 83.59 mg g-1, 61.51 mg g-1 and 40.67 mg g-1, respectively. Cr(VI) ions were bound to ferrihydrite in higher amounts then Cr(III) ions and the maximum adsorption capacity increased as the pH of the solution decreased and was 53.14 mg g-1 at pH 5.0 and 83.73 mg g-1 at pH 3.0. The adsorption process of Cr species was pH dependent, and the ions were bound to the surface of ferrihydrite by surface complexation. The Sips isotherm was the best-fit model to the results obtained from among the four isotherm models used, i.e., Freundlich, Langmuir, Dubinin-Radushkevich and Sips, indicating different adsorption centers participate in Cr uptake. In order to assess the bonding strength of the adsorbed chromium ions the modified BCR procedure, dedicated to the samples with a high iron content, was used. The results of the sequential extraction showed that Cr(III) ions were bound mainly in the immobile residual fraction and Cr(VI) ions were bound in the reducible fraction. The presence of Fe (oxyhydr)oxides in soil and sediments increases their adsorption capacity for Cr, in particular for hexavalent Cr in an acid environment due to their properties (high pHPZC).
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