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Synthesis and characterization of nanocrystalline mordenite, high silica zeolite RHO, and copper faujasite.

机译:纳米晶丝光沸石,高硅沸石RHO和八面沸石铜的合成与表征。

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摘要

Mordenite is a zeolite that has been used as a selective adsorbent and as a catalyst. In reactions where the diffusion of reagents into the pore system is the rate-determining step, nanoparticles of the catalyst improve the reaction rate. Mordenite with a crystal diameter smaller than 100 nm has been prepared by the modification of different synthetic parameters such as the source of aluminum, the presence of seeds, the use of low temperatures (150°C vs. 170°C), longer crystallization times (24 h vs. 96 h), and different silica to alumina ratios (10--30). The decrease in the crystal diameter of the prepared mordenite was monitored by the application of the Scherrer equation that relates the broadness of the X-ray diffraction peaks to crystal sizes.; Zeolite RHO with an initial silica to alumina ratio (SAR) higher than 20 has been prepared. EDTA, citric acid, and tartaric acid have been used as complexing agents in the synthesis of zeolite RHO. Crystallization time increases (from 48 h to 900 h) with increasing the silica to alumina ratios (SAR) of the initial gel (SAR: 10.8 to 30) and by adding complexing agents. Complexing agents favor the formation of small crystals (0.8 mum) with increased silica to alumina ratio (final SAR: 4.5 vs. 4.0 without complexing agents). The products were characterized by XRD, FESEM, EDX, FTIR, and in-situ XRD.; Copper containing faujasite has been successfully prepared for the first time using a direct synthesis method. Ammonium hydroxide was used to form a copper complex that was later mixed with the reacting gel. Crystallization took place at 85°C for 11 days. The copper containing faujasite obtained was characterized by XRD, FESEM, EDX, EPR, FTIR, TPR, and BET. According to the XRD pattern only FAU type zeolite was obtained. According to TPR experiments, the reduction temperature for Cu2+ ions present in Cu-FAU prepared by direct synthesis was 70 K higher than for Cu-FAU prepared by ion-exchange. This difference can be due to the different location of the copper ions in the supercages or in the sodalite cages of the faujasite.
机译:丝光沸石是已经用作选择性吸附剂和催化剂的沸石。在反应物扩散到孔隙系统中是决定速率的步骤的反应中,催化剂的纳米颗粒提高了反应速度。晶体直径小于100 nm的丝光沸石是通过修改不同的合成参数来制备的,例如铝的来源,晶种的存在,使用低温(150°C对170°C),更长的结晶时间(24小时vs. 96小时),以及不同的二氧化硅/氧化铝比例(10--30)。所制备的丝光沸石的晶体直径的减小是通过应用将X射线衍射峰的宽度与晶体尺寸相关的Scherrer方程来监测的。已经制备了初始二氧化硅与氧化铝之比(SAR)高于20的RHO沸石。 EDTA,柠檬酸和酒石酸已被用作合成沸石RHO的络合剂。结晶时间的增加(从48小时增加到900小时)随着初始凝胶的二氧化硅与氧化铝之比(SAR:10.8至30)的增加以及添加络合剂的增加。络合剂有利于形成小晶体(0.8微米),而二氧化硅与氧化铝的比例增加(不使用络合剂时最终SAR:4.5对4.0)。产物通过XRD,FESEM,EDX,FTIR和原位XRD表征。使用直接合成方法首次成功制备了含铜的八面沸石。使用氢氧化铵形成铜络合物,然后将其与反应凝胶混合。在85℃下结晶11天。通过XRD,FESEM,EDX,EPR,FTIR,TPR和BET对获得的含铜八面沸石进行表征。根据XRD图谱,仅获得FAU型沸石。根据TPR实验,通过直接合成制备的Cu-FAU中存在的Cu2 +离子的还原温度比通过离子交换制备的Cu-FAU高70K。这种差异可能是由于八面沸石的超笼或方钠石笼中铜离子的位置不同。

著录项

  • 作者单位

    University of Connecticut.;

  • 授予单位 University of Connecticut.;
  • 学科 Engineering Materials Science.
  • 学位 Ph.D.
  • 年度 2005
  • 页码 103 p.
  • 总页数 103
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 工程材料学;
  • 关键词

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