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首页> 外文学位 >Hydrogenation of nitriles on a well-characterized nickel surface: From surface science studies to liquid phase catalytic activity measurements.
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Hydrogenation of nitriles on a well-characterized nickel surface: From surface science studies to liquid phase catalytic activity measurements.

机译：表征良好的镍表面上的腈加氢：从表面科学研究到液相催化活性测量。

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摘要

The work described in this thesis is aimed at providing information about the mechanism and factors affecting the performance of nickel-based catalyst in nitrile hydrogenation reactions. The catalytic surface is modeled by a nickel single crystal surface which can be cleaned and characterized in an ultra-high vacuum environment. In the first part, the techniques of surface science are used to characterize the bonding of adsorbates and to identify surface intermediates which might play a role during the hydrogenation of nitriles. In the second part, liquid-phase hydrogenation reactions of olefins are carried out on a polycrystalline platinum foil prepared in UHV.;The adsorption of acetonitrile on Ni(111) leads to an ordered (2 x 2) overlayer. Low-energy electron diffraction (LEED) intensity vs. energy (I-V) curves for this structure have been measured and analysed using an automated search method based on the Tensor LEED approximation. The adsorbed acetonitrile is bonded to the surface by both carbon and nitrogen with the C-N axis almost parallel to the metal surface. The rehybridized acetonitrile on the surface is non-linear with a C-C-N angle estimated at 123;The bonding and geometry of methylamine ;The proposed dehydrogenation pathway of ethylamine was also examined by extended Huckel calculations. The binding energies of the decomposition products and intermediate surface species formed on Ni(111) from adsorption of ethylamine ;The thermal decomposition of these simple amines on Ni(111) produces a ;In order to correlate the liquid phase activity and selectivity of a catalytic surface with its structure and composition, we have built and tested the first liquid phase hydrogenation cell coupled to an ultra-high vacuum surface analysis chamber. This novel apparatus is tested with the hydrogenation of cyclohexene to cyclohexane on a polycrystalline platinum foil, and then with the hydrogenation of 1-hexene to n-hexane. The hydrogenation of propionitrile is also attempted but no activity is detected. Hydrogenations of olefins and nitriles were also carried out on Ni(111) but no products could be formed.;We finally review the techniques of surface science that have been applied to molecular level studies at both solid-gas and solid-liquid interfaces. (Abstract shortened by UMI.).
机译：本文所描述的工作旨在提供有关影响镍基催化剂在腈加氢反应中性能的机理和因素的信息。催化表面以镍单晶表面为模型，可以在超高真空环境中对其进行清洁和表征。在第一部分中，表面科学技术用于表征吸附物的键合并确定可能在腈加氢过程中起作用的表面中间体。在第二部分中，在UHV制备的多晶铂箔上进行烯烃的液相加氢反应。乙腈在Ni（111）上的吸附导致有序的（2 x 2）覆盖层。使用基于Tensor LEED近似的自动搜索方法，已经测量并分析了该结构的低能电子衍射（LEED）强度与能量（I-V）曲线。吸附的乙腈通过碳和氮结合到表面，C-N轴几乎平行于金属表面。表面再混合的乙腈是非线性的，C-C-N角估计为123；甲胺的键合和几何形状；还通过扩展的Huckel计算方法研究了拟议的乙胺脱氢途径。乙胺吸附后在Ni（111）上形成的分解产物和中间表面物质的结合能;这些简单胺在Ni（111）上的热分解产生一个C;为了关联液相活性和催化剂的选择性凭借其结构和组成，我们已经建造并测试了第一个与超高真空表面分析室相连的液相加氢池。通过在多晶铂箔上将环己烯氢化为环己烷，然后将1-己烯氢化为正己烷，对这种新型设备进行了测试。还尝试了丙腈的氢化，但未检测到活性。还对Ni（111）进行了烯烃和腈的加氢反应，但没有生成任何产物。我们最后回顾了应用于固体-气体和固-液界面的分子水平研究的表面科学技术。 （摘要由UMI缩短。）。

著录项

  • 作者

    Gardin, Denis Emmanuel.;

  • 作者单位

    University of California, Berkeley.;

  • 授予单位 University of California, Berkeley.;
  • 学科 Chemistry Physical.
  • 学位 Ph.D.
  • 年度 1993
  • 页码 189 p.
  • 总页数 189
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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