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1.
Spectroscopic investigation of oxygen vacancies in CeO[sub]2 : dissertation
Thanveer Thajudheen, 2021, doktorska disertacija

Opis: A unique material, ceria (CeO2), which is widely applied in automobile exhaust catalysts, is functional due to presence of defects in its crystal structure. Furthermore, the structural defects dictate electrical and chemical properties of ceria. The creation of intrinsic oxygen vacancies in ceria is responsible for oxygen-ion conductivity in solid oxide fuel cells. This unfolds the keen interest in ceria defects. Using the analytical technique cathodoluminescence spectroscopy (CLS) we can characterize ceria for its band gap and the defect states within the band gap. Since CLS has a high spatial resolution, high sensitivity to low concentration of defects and ability to obtain depth resolved information it is an obvious technique of choice. The first part of the thesis is an introduction to the topic and description of the experimental techniques. Importance of ceria as a multifaceted material finding applications in areas spanning from energy production and conversion to biomedical applications is detailed. CLS as a tool to understand defect-related optical properties and advancement in the CL detection systems are discussed. To study the relationship between local structure and its impact on CL emission spectra, an X-ray absorption spectroscopy techniques were used. The X-ray absorption near edge structure (XANES) and the Extended x-ray absorption fine structure (EXAFS) techniques are summarized. The second part discusses CL emission from ceria. Initially, CL emission from reduced ceria and its dependence on oxygen vacancy concentration are presented. The origin of emission was attributed to different configurations of the oxygen vacancies and polarons. The recent F center description in ceria was adopted here. The intriguing observation of CL emission quenching as a function of oxygen vacancy concentration was explained on the basis of a relative change in population of F centers in ceria. This demonstrated the relevance of local structure for the CL emission in ceria. In order to have a better understanding of the system, La-doped ceria was proposed as a model system. A precise control over the stoichiometry helped to achieve a desired oxygen vacancy concentration. The CL emission behavior, as observed in reduced ceria, was replicated in the case of La-doped ceria and the analysis revealed that F+ centers favor CL emission whereas F0 centers are disadvantageous. The local structure investigation using EXAFS analysis of both cations Ce and La (K-Edge) showed distortion from the fluorite symmetry and corroborated the F center description of oxygen vacancies in ceria. Our results provide an experimental evidence for F center description involving oxygen vacancies and polarons.
Ključne besede: ceria, cathodoluminescence spectroscopy, local structure distortion, EXAFS analysis, La doped ceria, luminescence quenching, F centers, dissertations
Objavljeno v RUNG: 25.11.2021; Ogledov: 2390; Prenosov: 103
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2.
An extracellular polymeric substance quickly chelates mercury(II) with N-heterocyclic groups
Franco Baldi, Michele Gallo, Salvatore Daniale, Dario Battistel, Claudia Faleri, Alojz Kodre, Iztok Arčon, 2017, izvirni znanstveni članek

Opis: A strain of Klebsiella oxytoca DSM 29614 is grown on sodium citrate in the presence of 50 mg l−1 of Hg as Hg(NO3)2. During growth, the strain produces an extracellular polymeric substance (EPS), constituted by a mixture of proteins and a specific exopolysaccharide. The protein components, derived from the outer membrane of cells, are co-extracted with the extracellular exopolysaccharide using ethanol. The extracted EPS contains 7.5% of Hg (total amount). This indicates that EPS is an excellent material for the biosorption of Hg2+, through chemical complexation with the EPS components. The binding capacity of these species towards Hg2+ is studied by cyclic voltammetry, and Hg L3-edge XANES and EXAFS spectroscopy. The results found indicate that Hg2+ is mainly bound to the nitrogen of the imidazole ring or other N-heterocycle compounds. The hydroxyl moities of sugars and/or the carboxyl groups of two glucuronic acids in the polysaccharide can also play an important role in sequestring Hg2+ ions. However, N-heterocyclic groups of proteins bind Hg2+ faster than hydroxyl and carboxyl groups of the polysaccharide.
Ključne besede: Klebsiella oxytoca, Biosorption, Proteins, Polysaccharide, Cyclic voltammetry, EXAFS analysis
Objavljeno v RUNG: 03.03.2017; Ogledov: 4561; Prenosov: 0
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