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Static and dynamic properties of Cn/Cu(001) surfaces and oxidation, dissociation and bimolecular decarboxylation of isocyanate species adsorbed on Cu(001)

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  1. Tez No: 402689
  2. Yazar: ERKAN ZİYA ÇİFTLİKLİ
  3. Danışmanlar: PROF. JANE HINCH
  4. Tez Türü: Doktora
  5. Konular: Kimya Mühendisliği, Chemical Engineering
  6. Anahtar Kelimeler: Belirtilmemiş.
  7. Yıl: 2012
  8. Dil: İngilizce
  9. Üniversite: Rutgers, The State University of New Jersey-New Brunswick Campus
  10. Enstitü: Yurtdışı Enstitü
  11. Ana Bilim Dalı: Belirtilmemiş.
  12. Bilim Dalı: Belirtilmemiş.
  13. Sayfa Sayısı: 176

Özet

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Özet (Çeviri)

This dissertation presents an outlines my investigations of static and dynamic properties of adsorbed cyanide (CN) and isocyanate (-NCO) species as well as some of their chemistries. Surface bound CN-containing species have not previously been studied extensively, partially due to the inapplicability of fundamental e-beam based surface analysis techniques for investigations. I had the opportunity in my studies to employ multiple surface probing techniques, i.e. HAS, XPS, NEXAFS, TPD and RAIRS, to compile and cross-examine information from CN, –NCO, and derived species, adsorbed on the Cu(001) surface. 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).

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