Oxygène

Résumé

L'oxygène est l'élément chimique de numéro atomique 8, de symbole O. C'est la tête de file du groupe des chalcogènes, souvent appelé groupe de l'oxygène. Découvert indépendamment en 1772 par le Suédois Carl Wilhelm Scheele à Uppsala, et en 1774 par Pierre Bayen à Châlons-en-Champagne ainsi que par le Britannique Joseph Priestley dans le Wiltshire, l'oxygène a été nommé ainsi en 1777 par le Français Antoine Lavoisier du grec ancien (« aigu », c'est-à-dire ici « acide »), et (« générateur »), car Lavoisier pensait à tort que : Une molécule de formule chimique , appelée communément « oxygène » mais « dioxygène » par les chimistes, est constituée de deux atomes d'oxygène reliés par liaison covalente : aux conditions normales de température et de pression, le dioxygène est un gaz, qui constitue 20,8 % du volume de l'atmosphère terrestre au niveau de la mer. L'oxygène est un non-métal qui forme très facilement des composés, notamment des oxydes, avec pratiquement tous les autres éléme

Source officielle

https://fr.wikipedia.org/wiki/Oxyg%C3%A8ne

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Nanocomposite coatings composed of two phases with atomically sharp phase boundaries, show interesting mechanical properties. These properties are often originating from their high interface to volume ratio. Composites of nanocrystalline titanium nitride (TiN) grains surrounded by a one to two monolayer thick interlayer of silicon nitride (Si3N4) show an enhanced nanohardness. The central theme of this thesis is concernedwith the interfacial properties of two-dimensional bilayer systems, which are used as model systems to describe the interfaces occurring in nanocomposite coatings. The systems under investigation are TiN interfaces in contact with silicon (Si), silicon nitride (Si3N4) and aluminum nitride (AlN). The primary tool used to analyze the interfaces of bilayer systems is X-ray Photoelectron Spectroscopy (XPS) with emphasis put on the shake-up feature of the Ti 2p photoelectron line. Shake-ups in TiN are observed as an additional peak on the lower binding energy side of the energy lines of the Ti 2p orbitals. Shake-ups are strongly influenced by valence electrons and electron density distributions. This makes them a powerful tool to probe the chemical and electronic structure of TiN interfaces. The aim of this study is to utilize the shake-up energy and its intensity to gain insight into interfacial structures and correlate their changes to interfacial polarization and macroscopic mechanical properties. Single crystalline (sc-) and oxygen-free TiN as well as oxygen-free bilayer systems were deposited by unbalanced magnetron sputtering and analyzed by Angle Resolved (AR-)XPS. Bilayer samples were deposited and their quality was controlled using X-ray diffraction (crystallinity), Rutherford back scattering (elemental composition), and atomic force microscopy (roughness). All XPS samples were fabricated, transfered and analyzed whilst maintaining ultra high vacuum. A precise and self-consistent XPS data processing method was developed to evaluate Ti 2p spectra. This method accounts for the correct photoelectron line shape, background subtraction and photoelectron peak area intensity. Binding energy, shake-up energy and intensity ratios of shake-ups taken frompristine TiN surfaces are precisely determined, and the influence of oxygen on the information content in peak positions and intensities was investigated. The shake-up energy and intensity of bulk sc-TiN and its origin of the shake-up are discussed. An analytical description for the XPS signal ratio of bilayer systems is derived to separate the interfacial signals from the bulk information. The results obtained by this analytical description are strongly influenced by the interface thickness that has been found to be proportional to the overlayer thickness. The revealed interface properties show a correlation between the shake-up intensity and the interface morphology, oxygen content, overlayer material and overlayer thickness. AR-XPS and X-ray Photoelectron Diffraction (XPD) results were used to interpret the crystalline structure of the different TiN/AlN and TiN/Si3N4 bilayer systems. AlN shows XPD patterns indicating a crystalline growth of AlN on sc-TiN. The electrically insulating AlN overlayer creates a charge accumulation at the TiN interface, which results in an enhanced shake-up intensity. XPD patterns of Si3N4 systems revealed a crystalline growth of Si3N4 in the first 0.6nm. The intensity of the diffraction patterns reduces with increasing Si3N4 overlayer thickness due to a change in the growth behavior from crystalline to amorphous structures. Si3N4 films show, in comparison to AlN, reduced interface charging and hence a lower shakeup intensity. The crystalline growth of Si3N4 in the initial stages is hindered in systems where a bias voltage is applied to the substrate during the deposition process. In contrast to the unbiased systems, which have crystalline interfacial structures, the biased systems no longer show XPD patterns due to a loss of crystallinity. Additionally the shake-up intensity of biased systems is thickness-independent, which is in contrast to unbiased systems. The difference in the shake-up intensity of biased and unbiased Si3N4 is explained by a different band gap of the Si3N4 structure in the first two monolayers. This thesis shows that the increase in the shake-up intensity is correlated to intrinsic and extrinsic interface charging. The obtained results, in combination with theoretical structure models from literature, show that in one to two monolayer thick interlayers a build-up of interface polarization is unlikely. The observed nanohardness enhancement in TiN/Si3N4 systems is explained with already known hardness effects.

EPFL2012

Chargement

Model-based scale-up of a continuously operated consolidated bioprocess based on a microbial consortium for the production of ethanol

David Béat Dempfle

This work demonstrated that consolidated bioprocessing is a promising concept for conversion of lignocellulose to ethanol at industrial scale. CBP offers great cost saving potential, is feasible to be operated continuously and may be scaled up due to extensive knowledge of the process from a chemical engineering point of view.Cost savings of up to 27.5% of the total costs compared to conventional bioethanol production from lignocellulose, as stated by a techno-economic assessment, make continuous CBP the strongest lever to reduce processing costs of lignocellulosic ethanol. A cost sensitivity analysis identified scale and yield as the main cost-pushers from a process point of view, whereas the price level of the plant location has the highest impact on the investment conditions.To prove the feasibility of continuous CBP, and therefore the mentioned cost savings, experiments with a maximum titer of 3.258±0.007 g/L, a productivity of 0.025 g/(Lh) and constant enzyme production over 750h were conducted. Furthermore, the continuous experiments showed that experiments with identical volumetric oxygen transfer rate k_L a, but different oxygen fluxes per membrane area, showed titer differences of ca. 80% (1.83 g/L vs 3.26 g/L) in favor of setups with the large membrane surface. A rigorous process model was developed for continuously operated CBP. 9 species were considered (oxygen, glucose, total concentration Trichoderma reesei, secondary mycelia concentration of T. reesei, enzymes, cellulose, cellobiose, yeast density and ethanol). 8 of these 9 species needed to be modelled spatially resolved to account properly for mass transfer limitations. The fungal biofilm thickness d_f was found to be a critical parameter with an optimum for every membrane configuration. Smaller d_f reduced the fungal biofilm volume and thus, the enzyme production and larger d_f increased the diffusion path length causing shortage in nutrient supply as well as lower enzyme concentrations in the bulk. The enzyme synthesis rate of the secondary mycelia was fitted by reducing it by ca. 40% (0.67 FPU/(mLd) vs 1.152 (FPU/(mL*d) compared to batch models.With the process model as centerpiece, a scale-up framework consisting of the model and a set of non-dimensional parameters was developed to scale CBP from 2.7L laboratory scale to 130L pilot scale. The majority of the non-dimensional parameters could be kept constant during scale-up as requested by the similarity paradigm. Necessary changes were simulated with the model. Again, the fungal biofilm thickness d_f proved to be a relevant parameter for scale-up considerations. In general, the relative loss of biofilm volume is compensated by longer residence times since the residence time has by far the least impact on the process economics.Finally, popular rate-controlled separation techniques were investigated regarding their potential with CBP, since they offer the potential to reduce yeast inhibition, to avoid separation limitations by the azeotrope and they are not bound to the vapor-liquid-equilibrium of highly diluted ethanol-water mixtures. However, most of the mechanisms fail to handle the solids of the fermentation broth. Pervaporation, being the most promising concept for in-situ product removal, would be a cost-saving alternative to distillation for batch operation, but is limited by an unfavorable vapor-liquid equilibrium due to low bulk concentrations during continuous operation.

EPFL2022

Chargement

Magnetization Reversal Dynamics in Ferromagnetic Semiconductors

Liza Herrera Diez

This thesis is dedicated to the study of the magnetization reversal dynamics in compressively strained (Ga,Mn)As and differently functionalized (Ga,Mn)As materials. In the first part the domain wall dynamics of pure (Ga,Mn)As/GaAs materials is in the focus. The changes in the magnetic anisotropy energy landscape occurring as a function of temperature are monitored in detail by different experimental techniques. These measurements provide the necessary information for the identification of the temperature ranges corresponding to different magnetic anisotropy regimes. Knowing the biaxial anisotropy and uniaxial anisotropy dominated regimes the dependence of the domain wall dynamics on the magnetic anisotropy landscape is studied. Critical changes in domain wall alignment observed by Kerr microscopy are found upon changing from biaxial to uniaxial anisotropy. These changes could be partially attributed to the tendency of the system to minimize magnetic free poles at the domain boundaries. To complement the space resolved studies of the magnetization reversal, magnetic time relaxation effects are addressed. In particular the magnetic aftereffect in (Ga,Mn)As/GaAs is studied in detail. The irreversible aftereffect is evidenced as a critical reduction of the domain wall velocity with time under a constant applied magnetic field below coercivity. This time relaxation is tracked as a function of both time and magnetic field. The measurements show that the overall relaxation is composed of two relaxation processes acting in parallel at short and long time scales. By fitting these experimental results the values of the relaxation times of both relaxation processes were obtained. By this modeling also the values of the activation volumes for two independent (Ga,Mn)As materials are estimated. In the second part of this thesis the possibilities of tuning the electrical and magnetic properties of (Ga,Mn)As by volume and surface treatments are explored. As for the volume modification, oxygen species were incorporated into the (Ga,Mn)As films by means of exposure to an oxygen plasma. The incorporation of oxygen was evidenced by depth profile X-ray photoelectron spectroscopy. This treatment is found to weaken the ferromagnetism, visible as a reduction in the Curie temperature, and to hinder the electrical transport evidenced as an increase in the electrical resistance. In agreement with theories accounting for the hole mediated ferromagnetism in (Ga,Mn)As this behaviour was related to a hole compensation mechanism arising from the presence of oxygen impurities sitting in interstitial positions of the (Ga,Mn)As Zinc blende structure. In the last part, the modulation of the electrical and magnetic properties via surface functionalization is presented. The effects produced by the adsorption of molecular species on (Ga,Mn)As are similar to those found after oxygenation, namely a strong weakening of the magnetic properties and an increase in the values of the electrical resistance. However, in this case the distinctive feature is provided by the possibility of regulating the hole quenching effect by exploiting the additional degree of freedom provided by the chemical properties of the adsorbates. The adsorbate chosen for these experiments are dye molecules that absorb light in the visible range, in this way allowing for a light modulated interaction with the substrate. Using this concept is was possible to observe a modulation of the ferromagnetic transition temperature, the coercive field and the electrical resistance upon illumination. These observations provide a proof of principle for the realization of photo-sensitized (Ga,Mn)As devices where the magnetic properties can be regulated by light.

EPFL2011

Chargement

EPFL2012

Model-based scale-up of a continuously operated consolidated bioprocess based on a microbial consortium for the production of ethanol

David Béat Dempfle

EPFL2022

Magnetization Reversal Dynamics in Ferromagnetic Semiconductors

Liza Herrera Diez

EPFL2011