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The formation and properties of silver and iron nanoscale components in the Ag-Fe bimetallic system deposited on mordenite depend on several parameters during their preparation. Previously, it was shown that an important condition for optimizing nano-center properties in a bimetallic catalyst is to change the order of sequential deposition of components; the order "first Ag+, then Fe2+" was chosen as optimal. In this work, the influence of exact Ag/Fe atomic proportion on the system's physicochemical properties was studied. This ratio has been confirmed to affect the stoichiometry of the reduction-oxidation processes involving Ag+ and Fe2+, as shown by XRD, DR UV-Vis, XPS, and XAFS data, while HRTEM, SBET and TPD-NH3 show little change. However, it was found the correlation between the occurrence and amount of the Fe3+ ions incorporated into the zeolite's framework and the experimentally determined catalytic activities towards the model de-NOx reaction along the series of nanomaterials elucidated in this present paper.
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Mordenite is a well-known zeolite widely used for industrial processes. However, its pore architecture can be inconvenient due to diffusional issues. A study of the synthesis parameters from an organic-free dense gel was carried out to control the crystal morphology, which resulted in finned mordenite zeolite particles. The obtained materials were characterized by XRD, FTIR, 29Si and 27Al MAS-NMR, elemental analysis, nitrogen physisorption, SEM, and TEM. We found that careful manipulation of the hydrothermal parameters directly affected the sizes and morphologies of the crystallites and particles, as well as the textural properties of the final products. Additionally, it was found that mordenite could exhibit a fin morphology with additional mesoporosity, which is a promising means to reduce the diffusional problems of one-dimensional-channel zeolites.
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The present study evaluates the feasibility of partially dealuminated natural mordenite as a catalyst support by studying improvement in its textural properties. This is the first study that reports the dealumination of natural zeolite-based tuffs from Ecuador. For this purpose, mordenite-rich tuffs were obtained from deposits close to Guayaquil, Ecuador. The raw material was micronized in order to increase its surface, and treated with NH4Cl. NH4+ cation-exchanged samples were finally reacted with HCl(aq) to complete the dealumination process. The partially dealuminated samples were characterized using techniques such as XRD, FT-IR, SEM-EDS, and identification of their textural properties. Dealumination with HCl(aq) increased the Si/Al ratio up to 9 and kept the crystallographic structure of natural mordenite, as XRD results showed that the structure of mordenite was not altered after the dealumination process. On the other hand, textural properties such as surface area and microporosity were improved as compared to natural mordenite. In view of these results, the feasibility of using natural mordenite as a catalyst support is discussed in this study.
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Multimetallic systems, instead of monometallic systems, have been used to develop materials with diverse supported species to improve their catalytic, antimicrobial activity, etc., properties. The changes in the types of nanospecies obtained through the thermal reduction of ternary Ag+-Cu2+-Zn2+/mordenite systems in hydrogen, followed by their cooling in an air or hydrogen atmosphere, were studied. Such combinations of trimetallic systems with different metal content, variable ratios (between them), and alternating atmosphere types (during the cooling after reducing the samples in hydrogen at 350 °C) lead to diversity in the obtained copper and silver nanospecies. No reduction of Zn2+ was evidenced. A low silver content leads to the formation of reduced silver clusters, while the formation of nanoparticles of a bigger size takes place in the trimetallic samples with high silver content. The cooling of the reduced trimetallic samples in the air causes the oxidation of the obtained metallic clusters and silver and copper nanoparticles. In the case of copper, such conditions lead to the formation of mainly copper (II) oxide, while the silver nanospecies are converted mainly into clusters and nanoparticles. The zinc cations provoked changes in the mordenite matrix, which was associated with the formation of point oxygen defects in the mordenite structure and the formation of surface zinc oxide sub-nanoparticles in the samples cooled in the air.
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This work describes the newly discovered zeolites in the eastern region of Cuba. In the researched area, there have been no previous studies of natural zeolite exploration. Therefore, the results shown here are new. The main object of this research is to analyse five samples of zeolites and demonstrate their pozzolanic capacity and the possibility of their usage in the industrial manufacturing of pozzolanic cements. The study of the samples was performed by X-ray diffraction (XRD), X-ray fluorescence (XRF) and scanning electron microscopy (SEM). A chemical analysis (CAQ) to determine the quality of the samples as pozzolans was performed, by determining the total SiO2, reactive SiO2, total CaO, reactive CaO, Al2O3, MgO and the insoluble residue (I.R.). Lastly, an eight-day pozzolanicity analysis (PA) was carried out to determine the pozzolanic reactivity of the samples. The results obtained by XRD, XRF and SEM established that the researched zeolite samples have two main zeolitic phases: mordenite and clinoptilolite. Altered volcanic glass, quartz and smectite (montmorillonite) are the secondary phases. The results of the chemical quality analysis (CAQ) showed that the samples contain a considerable amount of reactive SiO2 and reactive CaO, as well as a low content of insoluble residue, which reinforces their properties as pozzolans. The results of the pozzolanicity analysis (PA) concluded that the analysed samples actively react with Ca(OH)2 after eight days. Based on all the results mentioned above, it is established that both mordenite and clinoptilolite behave like pozzolans and can be recommended for the manufacture of pozzolanic cements, which have more effective properties than Portland cement, in terms of physical, chemical and mechanical strength, low heat of hydration, resistance to sulphates, low CO2 emissions to the atmosphere and negligible impacts on the environment.
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Helicobacter pylori can be found in the stomach of about half of the humans, and a large population can be associated with serious diseases. To survive in the stomach H. pylori increases the pH locally by producing ammonia which binds to H+ becoming ammonium. This work investigated the effects on the in-vitro growth of H. pylori of a natural cation-exchanger mainly composed (≈70%) of clinoptilolite and mordenite. The zeolitized material from Cuba was evaluated in its original form (M), as well as in its Na- (M-Na) and Zn-exchanged (M-Zn) counterparts. In the preliminary agar cup diffusion test, H. pylori revealed susceptibility only to M-Zn, with a direct relationship between concentration and width of inhibition halo. Further experiments evidenced that bacterium replication increases when ammonium is supplied to the growth medium and decreases when zeolites subtract NH4+ via ion exchange. Due to the multi-cationic population of its zeolites M was not effective enough in removing ammonium and, in the Minimum Inhibitory Concentration (MIC) test, allowed bacterial growth even at a concentration of 50 mg/mL. Inhibition was achieved with M-Na because it contained sodium zeolites capable of maximizing NH4+ subtraction, although the MIC was high (30 mg/mL). M-Zn evidenced a more effective inhibitory capacity, with a MIC of 4 mg/mL. Zinc has antimicrobial properties and H. pylori growth was affected by Zn2+ released from clinoptilolite and mordenite. These zeolites, being more selective towards NH4+ than Zn2+, can also subtract ammonium to the bacterium, thus enhancing the efficacy of M-Zn.
Assuntos
Silicatos de Alumínio/farmacologia , Antibacterianos/farmacologia , Helicobacter pylori/efeitos dos fármacos , Zeolitas/farmacologia , Zinco/farmacologia , Silicatos de Alumínio/química , Compostos de Amônio/metabolismo , Compostos de Amônio/farmacologia , Antibacterianos/química , Cuba , Helicobacter pylori/crescimento & desenvolvimento , Troca Iônica , Testes de Sensibilidade Microbiana , Sódio/química , Zeolitas/química , Zinco/químicaRESUMO
Two different natural zeolites from Cuba and Mexico, which are already being used as contemporaneous drugs or dietary supplements in Germany and Mexico, respectively, are applied in a comparative study of their histamine-binding capacities as a function of their particle sizes. The zeolites are characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM) and N2-sorption measurements (BET surface areas). The Cuban zeolite contains clinoptilolite and mordenite as major phases (78% zeolite), whereas the Mexican one contains only clinoptilolite (65% zeolite). Both zeolites are apparently free from fibrous materials according to SEM. Both zeolites adsorb significant amount of histamine under the experimental conditions. Nevertheless, the results showed that the histamine-binding capacity of the Cuban zeolite is higher than the Mexican one and the smaller the particle size of zeolite, the higher the histamine-binding capacity. This difference could be due to the variation in their mineralogical compositions resulting in varied BET surface areas. Thus, the high histamine-binding capacities of Cuban zeolites seem to be due at least partly to the presence of the large-pore zeolite mordenite, providing high total pore volumes, which will be discussed in detail. For the first time, we have shown that the mineralogical compositions of natural zeolites and their particle sizes play a key role in binding histamine, which is one of the most important regulators in human physiology.