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首页> 外文学位 >Static and dynamic properties of cyanide/copper(001) surfaces and oxidation, dissociation and bimolecular decarboxylation of isocyanate species adsorbed on copper(001).
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Static and dynamic properties of cyanide/copper(001) surfaces and oxidation, dissociation and bimolecular decarboxylation of isocyanate species adsorbed on copper(001).

机译：氰化物/铜（001）表面的静态和动态特性，以及吸附在铜（001）上的异氰酸酯类物质的氧化，解离和双分子脱羧。

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摘要

While angle resolved He atom scattering (HAS) was employed to identify and investigate the ordered superstructure of CN/Cu(001) surfaces, TOF-HAS was employed to investigate its dynamic properties. The CN/Cu(001) surface induced unprecedented simultaneous coherent He diffraction with a large "classical" multiphonon backscattered He intensity. A superstructure is implied that contains both rigidly bound CN species, which maintain the long range c(10x6) translational symmetry, together with bound highly-dynamic CN species that exhibit large thermally induced displacements. The NEXAFS measurements suggest multiple spatial binding configurations for the adsorbed CN moieties. In addition, TPD spectra of C2N2 desorption from CN/Cu(001) surface were analyzed, using my newly developed method, to determine the activation energies for desorption as a function of CN coverage.;There are two reactions of NCO species examined in my studies. The first is the newly discovered mutual reaction between NCO species. This type of interaction had not been seen before, as it is essentially difficult to prepare pure NCO/metallic surfaces. Copper was chosen as a substrate as HNCO exposures of Cu(001) at RT, followed by spontaneous H2 desorption, do produce NCO only surfaces. A thermal treatment of the surface, at 573K, leads to a bimolecular decarboxylation of NCO, leaving a carbodimide species (NCN) on the surface. The sp-hybridized linear NCN moieties, which are bound nearly parallel to the substrate, show high thermal stability. The second reaction of NCO, which I have studied, is its oxidation. In particular, the effect of CN coadsorbates on the oxidation of NCO was studied. It was found that the presence of CN catalyzes a dissociation reaction of NCO species on Cu(001).
机译：角度分辨He原子散射（HAS）用于识别和研究CN / Cu（001）表面的有序超结构，而TOF-HAS用于研究其动态特性。 CN / Cu（001）表面引起了空前的同时相干He衍射，并具有大的“经典”多声子反向散射He强度。隐含着一个上部结构，它既包含刚性结合的CN物种，保持长距离c（10x6）平移对称性，又包含表现出大的热诱导位移的结合的高动态CN物种。 NEXAFS测量结果表明，所吸附的CN部分具有多种空间结合构型。此外，使用我最新开发的方法分析了CN / Cu（001）表面脱附的C2N2的TPD光谱，以确定脱附的活化能随CN覆盖率的变化。学习。首先是新发现的NCO物种之间的相互反应。以前从未见过这种相互作用，因为制备纯的NCO /金属表面非常困难。选择铜作为基材，是因为在室温下H（3）对Cu（001）的HNCO暴露，然后自发解吸H2，确实会产生仅NCO的表面。在573K处对表面进行热处理会导致NCO发生双分子脱羧，从而在表面上留下碳二亚胺类（NCN）。几乎平行于底物结合的sp杂化线性NCN部分显示出高的热稳定性。我研究的NCO的第二个反应是其氧化。特别地，研究了CN共吸附物对NCO氧化的影响。发现CN的存在催化NCO物质在Cu（001）上的离解反应。

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  • 作者

    Ciftlikli, Erkan Ziya.;

  • 作者单位

    Rutgers The State University of New Jersey - New Brunswick.;

  • 授予单位 Rutgers The State University of New Jersey - New Brunswick.;
  • 学科 Chemistry Physical.;Engineering Materials Science.;Physics Condensed Matter.;Physics Molecular.
  • 学位 Ph.D.
  • 年度 2012
  • 页码 176 p.
  • 总页数 176
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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