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1.
Optical properties of near-surface urban aerosols and their chemical tracing in a Mediterranean city (Athens)
Dimitris Katsanos, Aikaterini Bougiatioti, Eleni Liakakou, Dimitris G. Kaskaoutis, Iasonas Stavroulas, D. Paraskevopoulou, Maria Lianou, Basil E. Psiloglou, Evangelos Gerasopoulos, Christodoulos Pilinis, 2019, izvirni znanstveni članek

Opis: One-year measurements (October 2016–September 2017) of aerosol optical properties in the Athens urban environment were analyzed; for closure purposes, the results were supported by data of chemical composition of the non-refractory submicron aerosol fraction acquired with an Aerosol Chemical Speciation Monitor (ACSM). Both the spectral scattering (bsca) and absorption (babs) coefficients exhibit a pronounced annual variability with higher values (63.6 Mm–1 at 550 nm and 41.0 Mm–1 at 520 nm, respectively) in winter, due to domestic heating releasing increased carbonaceous emissions and the shallow mixing layer trapping aerosols near the surface. Much lower values (33.5 Mm–1 and 22.9 Mm–1 for bsca and babs, respectively) are found during summer, indicating rather aged aerosols from regional sources. The estimations of the dry spectral single scattering albedo (SSA), scattering (SAE) and absorption (AAE) Ångström exponents focus on the seasonality of the urban aerosols. The high SAE (~2.0) and low SSA (0.62 ± 0.11) values throughout the year indicate the dominance of fine-absorbing aerosols from fossil-fuel combustion, while the high AAE (~1.5) in winter suggests enhanced presence of biomass-burning aerosols. Pronounced morning and late evening/night peaks are found in both bsca and babs during winter, coinciding with the morning traffic rush hour and increased residential wood burning in the evening, while in the other seasons, the diurnal patterns flatten out. The wind speed strongly affects the aerosol loading and properties in winter, since for winds below 3 m s–1, a high increase in bsca and babs is observed, consistent with low dilution processes and hazy/smoggy conditions. Our closure experiments indicate a good agreement (R2 = 0.91, slope = 1.08) between the reconstructed and measured bsca values and reveal that organic matter contributes about half of the sub-micron mass in winter, followed by sulfate (~40%) and nitrate (10%, only in winter) aerosols.
Ključne besede: urban aerosols, light scattering, absorption, chemical species, wood burning, Athens
Objavljeno v RUNG: 10.05.2024; Ogledov: 401; Prenosov: 2
.pdf Celotno besedilo (1,36 MB)
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2.
Amorphous nanocomposite of polycarbosilanes and aluminum oxide
Andraž Mavrič, 2018, doktorska disertacija

Opis: This work presents a paradigm for high temperature stabilization of bulk amorphous aluminium oxide. The thermodynamic stabilization is achieved by preparing a nanocomposite, where polymethylsilane dendritic molecules are dispersed in an aluminium hydroxide gel. Upon heat-treatment the gel transforms to the amorphous aluminium oxide that is stable up to 900°C. The dispersion of the macromolecules and their covalent bonding to the alumina matrix induce homogeneously distributed strain fields that keep the alumina amorphous. The first part of the thesis focuses on the synthesis, characterization and solubility properties of the dendritic polymethylsilane. The polymethylsilane is synthetized by electrochemical polymerization from trichloromethylsilane monomer. The polymerization mechanism, involving a single polymerization pathway, is identified. The polymer growth proceeds through reduction of the monomers to the silyl anions and their addition to the growing polymer. The solubility of three chemically related but topologically different polysilanes (linear, dendritic and network) were studied by dynamic light scattering. At room temperature the agglomerates in a range from 500 to 1300 nm are present. They undergo de-agglomeration at slightly elevated temperatures of around 40°C. The de-agglomeration results in formation of stable solutions, where a hydrodynamic diameter of the individual polymer molecules was measured to be in a range from 20 to 40 nm. The obtained diameters of two dendritic polymethylsilane macromolecules, synthesized under different electrolysis conditions, are much larger than the theoretical size estimated for an ideal dendrimer. We determined by 29Si NMR that the reason for this is in a large number of branching irregularities (defects) contained in the molecular structure. Combining the experimental values obtained by DLS and density measurements with a structural model that considers the branching irregularities, it is shown that the inclusion of the defects allows the dendritic polymer to exceed the sterical limitations and form the hyperbranched dendritic structure. The final size depends on a relative amount of the branching defects. In the second part, the synthetized polymethylsilane molecules were successfully used for the nanocomposite formation. The aluminium hydroxide gel with the dispersed polymethylsilane molecules was prepared as a precursor. Upon heat-treatment it gives the amorphous aluminium oxide stable up to 900°C. The dispersed macromolecules induce homogeneously distributed strain fields that keep the aluminium oxide amorphous during the thermal treatment the dispersed macromolecules covalently bind to the matrix, inducing the interface strain. The amorphous state was confirmed by the presence of penta-coordinated aluminium detected by 27Al NMR and a low bandgap measured by UV-vis absorption spectroscopy.
Ključne besede: amorphous aluminium oxide, polymethylsilane, nanocomposite, electropolymerization, solubility, agglomeration, de-agglomeration, dendrimer, hyperbranched dendritic structure, dynamic light scattering, thermal analysis, transmission electron microscopy, scanning electron microscopy, X-ray diffraction, infrared spectroscopy, UV-Vis spectroscopy
Objavljeno v RUNG: 19.07.2018; Ogledov: 6603; Prenosov: 218
.pdf Celotno besedilo (5,07 MB)

3.
Polymer Nanoparticle Sizes from Dynamic Light Scattering and Size Exclusion Chromatography: The Case Study of Polysilanes.
Artem Badasyan, Andraž Mavrič, Irena Kralj Cigić, Tim Bencik, Matjaž Valant, 2018, izvirni znanstveni članek

Opis: Dynamic Light Scattering (DLS) and Size Exclusion Chromatography (SEC) are among the most popular methods for determining polymer sizes in solution. Taking dendritic and network polysilanes as a group of least soluble polymer substances, we critically compare and discuss the difference between nanoparticle sizes, obtained by DLS and SEC. Polymer nanoparticles are typically in poor solution conditions below the theta point and are in globular conformation therefore. Determination of particle sizes in presence of attractive interactions is not a trivial task. The only possibility to measure aggregation-free, a true molecular size of polymer nanoparticles in such regime of solution, is to operate with the dilute solution of globules (below theta point and above the miscibility line). Basing on results of our polysilane measurements, we come to a conclusion that DLS provides more reliable results than SEC for the dilute solution of globules. General implications for the size measurements of polymer nanoparticles in solutions are discussed.
Ključne besede: Polymer Nanoparticle, Dynamic Light Scattering, Size Exclusion Chromatography, Polysilanes
Objavljeno v RUNG: 16.05.2018; Ogledov: 4614; Prenosov: 16
.pdf Celotno besedilo (3,17 MB)

4.
Efficient de-agglomeration of polysilane macromolecules in solution and their molecular size
Andraž Mavrič, Artem Badasyan, Mattia Fanetti, Matjaž Valant, 2017, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: polysilane, solubility, de-agglomeration, dynamic light scattering
Objavljeno v RUNG: 03.07.2017; Ogledov: 4810; Prenosov: 0
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5.
Temperature induced de-agglomeration of the polysilane macromolecules
Andraž Mavrič, Artem Badasyan, Mattia Fanetti, Matjaž Valant, 2016, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: polysilane, de-agglomeration, dynamic light scattering, differential scanning calorimetry
Objavljeno v RUNG: 05.10.2016; Ogledov: 5479; Prenosov: 0
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