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Theoretical investigation of H2 generation systems: From homogenous to heterogeneous photo-catalysis

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  1. Tez No: 508555
  2. Yazar: YELİZ GÜRDAL DURĞUN
  3. Danışmanlar: Prof. JURG HUTTER
  4. Tez Türü: Doktora
  5. Konular: Enerji, Su Ürünleri, Energy, Aquatic Products
  6. Anahtar Kelimeler: Belirtilmemiş.
  7. Yıl: 2017
  8. Dil: İngilizce
  9. Üniversite: Universität Zürich
  10. Enstitü: Yurtdışı Enstitü
  11. Ana Bilim Dalı: Belirtilmemiş.
  12. Bilim Dalı: Belirtilmemiş.
  13. Sayfa Sayısı: 146

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Özet (Çeviri)

In the quest of renewable sources of energy one of the most promising solution is the production of molecular hydrogen from water activated by solar energy. The photoinduced reactive cycle to split water and generate H2 with a clean and sustainable process relies on the choice of ecient photo-catalysts for both the oxidation and the reduction steps. Recent studies revealed that molecules with Cobalt (Co) active centers might achieve a commercially reasonable eciency in reducing water, thus being candidates for the replacement of expensive transition metals, such as Platinum and Ruthenium. In this respect, we investigate H2 production systems based on Co centered poly-pyridyl complexes in homogeneous and heterogeneous environments using density functional theory and ab-initio molecular dynamics. Concerning the homogeneous catalysis, we explore a few di erently ligated Cobased catalysts immersed in water solution. The emphasis is on the e ects of structural features, i.e. the number of the pyridyl subunits, exibility of the ligands, and coordination sphere around Co to understand the role of these structural features on the catalysts activity towards H2 production. Heterogeneous systems, instead, are grouped in two sections: oxide and metal surfaces where the Co-based water reduction catalysts are immobilized. The adsorption of both the bare ligand and the Co-metalated poly-pyridyl complexes and their assemblies on stoichiometric rutile TiO2(110) and reconstructed Au(111) surfaces are investigated. The optimized adsorption geometries, the e ects of Co insertion on the stability, molecule/surface and intermolecular interactions, electronic properties, their potential usage as H2 production systems are discussed for the two cases. In the case of Au(111) surface, we also address the role of herringbone reconstruction on the adsorption strength and on the modi cation of the molecular properties. Besides, rearrangements within the monolayer upon metalation and the possible intermediate states that hinder the metalation process are investigated.

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