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Nanocrystalline Zeolites: Synthesis, Mechanism, and Applications.

机译:纳米晶沸石:合成,机理和应用。

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摘要

Nanocrystalline zeolite particles are becoming an important material in many technical applications (e.g. zeolite membranes). Synthetic methods that minimize the zeolite crystal diameter, while providing a narrow particle size distribution, are of primary importance in these technical applications. However, there are several limitations to currently existing synthetic routes aimed at producing nanozeolites and zeolite membrane devices. For example, zeolite growth in these contexts typically requires days to weeks at high temperature to crystallize. Despite excellent performance of zeolite membranes in several separation applications, the long synthesis times required undermine any practical application of these technologies. This work focuses on chemical manipulation of zeolite nucleation processes in sol gel systems in effort to address such limitations. The primary findings indicate that careful control of the nucleation stage of a clear zeolite synthesis (optically transparent sol gel) allow the formation of zeolite Y nanocrystals less than 50 nm in diameter with a polydispersity index less than 0.2. Furthermore, chemical perturbations made during the nucleation stage of zeolite Y hydrogel synthesis is shown to accelerate crystal growth by a factor of 3-4, depending on the specific sol gel chemistry. These findings are applied to the nanocrystal seeding and rapid hydrothermal growth of zeolite Y membranes on inexpensive polymeric supports. A novel synthetic method is developed to this end. Also, the chemical and physical properties of monodisperse nanocrystalline zeolite Y synthesized herein are explored by electrochemical impedance spectroscopy. It is found that the particle interface plays an important role in the ionic conductivity of nanocrystalline zeolites in contrast to their larger zeolite counterparts in analogy to other ceramic and metal oxide ion conductors. Finally, the possibility to produce novel organic and inorganic composite systems through zeolite host-guest chemistry is explored. A nanozeolite-silver nanoparticle host-guest system is synthesized and a mechanism describing its evolution is developed. Also, the photochemistry of a colloidal nanozeolite-organic dye host-guest system is explored with ultrafast transient UV-Vis absorption spectroscopy. This allows some of the fastest chemical events to be probed within the host-guest system.
机译:纳米晶沸石颗粒在许多技术应用(例如沸石膜)中正成为重要的材料。在这些技术应用中,最重要的是使沸石晶体直径最小的合成方法,同时提供窄的粒度分布。但是,目前用于生产纳米沸石和沸石膜装置的合成路线存在一些限制。例如,在这些情况下,沸石的生长通常需要几天至几周的高温才能结晶。尽管沸石膜在多种分离应用中具有优异的性能,但所需的长合成时间破坏了这些技术的任何实际应用。这项工作集中于解决溶胶凝胶系统中沸石成核过程的化学操作,以解决此类限制。主要发现表明,对透明沸石合成(光学透明溶胶凝胶)的成核阶段的仔细控制允许形成直径小于50 nm,多分散指数小于0.2的沸石Y纳米晶体。此外,根据特定的溶胶凝胶化学性质,在沸石Y水凝胶合成成核阶段产生的化学扰动可将晶体生长加快3-4倍。这些发现被应用于廉价的聚合物载体上的Y晶体沸石的纳米晶种和快速水热生长。为此目的,开发了一种新颖的合成方法。另外,通过电化学阻抗谱研究了本文合成的单分散纳米晶体沸石Y的化学和物理性质。已经发现,与它们的较大的沸石对应物相比,与其他陶瓷和金属氧化物离子导体类似,颗粒界面在纳米晶沸石的离子电导率中起重要作用。最后,探讨了通过沸石客体化学方法生产新型有机和无机复合体系的可能性。合成了纳米沸石-银纳米颗粒客体系统,并描述了其演化机理。此外,胶体纳米沸石-有机染料主体-客体系统的光化学是用超快速瞬态UV-Vis吸收光谱法研究的。这样可以在来宾系统中探测某些最快的化学事件。

著录项

  • 作者

    Severance, Michael Andrew.;

  • 作者单位

    The Ohio State University.;

  • 授予单位 The Ohio State University.;
  • 学科 Chemistry Inorganic.;Nanotechnology.
  • 学位 Ph.D.
  • 年度 2014
  • 页码 369 p.
  • 总页数 369
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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