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Dissertations / Theses on the topic 'Autocatalytic'

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Published: 4 June 2021
Last updated: 20 February 2023

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1

Izzard, Michael. "Autocatalytic deposition of composite coatings." Thesis, Aston University, 1987. http://publications.aston.ac.uk/11907/.

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The deposition and properties of electroless nickel composite coatings containing graphite, PTFE and chromium were investigated. Solutions were developed for the codeposition of graphite and chromium with electroless nickel. Solutions for the deposition of graphite contained heavy metal ions for stability, with non-ionic and anionic surfactants to provide wetting and dispersion of the particles. Stability for the codeposition of chromium particles was achieved by oxidation of the chromium. Thin oxide layers of 200 nm thick prevented initiation of the electroless reaction onto the chromium. A mechanism for the formation of electroless composite coatings was considered based on the physical adsorption of particles and as a function of the adsorption of charged surfactants and metal cations from solution. The influence of variables such as particle concentration in solution, particle size, temperature, pH, and agitation on the volume percentage of particles codeposited was studied. The volume percentage of graphite codeposited was found to increase with concentration in solution and playing rate. An increase in particle size and agitation reduced the volume percentage codeposited. The hardness of nickel-graphite deposits was found to decrease with graphite content in the as-deposited and heat treated condition. The frictional and wear properties of electroless nickel-graphite were studied and compared to those of electroless nickel-PTFE. The self-lubricating nature of both coatings was found to be dependent on the ratio of coated area to uncoated area, the size and content of lubricating material in the deposit, and the load between contacting surfaces. The mechanism of self-lubrication was considered, concluding that graphite only produced an initial lubricating surface due to the orientation of flakes, unlike PTFE, which produced true self-lubrication throughout the coating life. Heat treatment of electroless nickel chromium deposits at 850oC for 8 and 16 hours produced nickel-iron-chromium alloy deposits with a phosphorus rich surface of high hardness. Coefficients of friction and wear rates were intially moderate for the phosphorus rich layer but increased for the nickel-iron-chromium region of the coating.
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2

Sullivan, Anne M. "Autocatalytic electroless gold deposition at low pH." Diss., Georgia Institute of Technology, 1995. http://hdl.handle.net/1853/10079.

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3

Agliari, Elena, Raffaella Burioni, Davide Cassi, and Franco M. Neri. "Autocatalytic reaction-diffusion processes in restricted geometries." Universitätsbibliothek Leipzig, 2016. http://nbn-resolving.de/urn:nbn:de:bsz:15-qucosa-192966.

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4

Agliari, Elena, Raffaella Burioni, Davide Cassi, and Franco M. Neri. "Autocatalytic reaction-diffusion processes in restricted geometries." Diffusion fundamentals 7 (2007) 1, S. 1-8, 2007. https://ul.qucosa.de/id/qucosa%3A14157.

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5

Arsene, Simon. "Pre-evolutionary dynamics in autocatalytic RNA networks." Thesis, Sorbonne Paris Cité, 2018. http://www.theses.fr/2018USPCC156/document.

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Les réseaux de molécules interdépendantes sont depuis quelque temps considérés comme de potentiels candidats pour avoir amorcé la transition de la biologie à la chimie. Bien qu'ils aient été intensivement examinés en théorie, il n'existe toujours aucune preuve expérimentale pour confirmer ou infirmer leur supposé rôle crucial dans les origines de la vie. En particulier, il nous manque encore une démonstration empirique des trois ingrédients habituellement présentés comme requis pour l'évolution darwinienne: l'hérédité, la variation et la sélection. Un système qui posséderait les trois tout en étant couplé à un processus de réplication en compartiments serait théoriquement capable d’évoluer au sens darwinien du terme. Par exemple, cela a été montré théoriquement pour les Ensembles Collectivement Autocatalytiques (CAS pour Collectively Aucatalytic Sets en anglais) où chaque molécule de l'ensemble est formée catalytiquement par un autre membre de l'ensemble. Ici, nous utilisons le système de ribozyme Azoarcus, qui catalysent des réactions de recombinaisons, pour former expérimentalement des CASs structurellement divers afin d’explorer leurs propriétés évolutives. Dans ce système, les ribozymes peuvent catalyser la formation d'autres ribozymes à partir de fragments plus petits, présents dans l'environnement. Nous utilisons un dispositif de microfluidique en gouttes associé au séquençage haut-débit pour mener une étude à grande échelle sur des milliers de CASs Azoarcus. Nous développons une approche perturbative pour identifier les paramètres topologiques importants contrôlant les variations observées dans les CAS à la suite de perturbations de l’environnement, ici l'ajout d'une nouvelle espèce. Nous déterminons ensuite l’ensemble restreint de caractéristiques du réseau régissant la mémoire des conditions initiales dans les CASs Azoarcus, un prérequis pour l'hérédité, en utilisant un modèle théorique validé par des données expérimentales. Enfin, nous démontrons qu’il existe dans les CASs Azoarcus des processus cataboliques qui les rendent robustes aux perturbations des fragments qui composent leur substrat et donc plus pertinent d’un point de vue prébiotique. Ces résultats démontrent le rôle crucial des CASs à base d’ARN dans les origines de la vie et illustrent comment la structure de leur réseau peut être adaptée pour obtenir des CASs avec des propriétés intéressantes d’un point de vue évolutif, ouvrant la voie à une démonstration expérimentale de l'évolution darwinienne avec système purement moléculaire
Networks of interdependent molecules are considered plausible candidates for initiating the transition from biology to chemistry. Though they have been intensively scrutinized theoretically, there is still no experimental evidence for confirming or denying their supposed crucial role in the origins of life. In particular, we are still lacking experimental proofs of any of the three ingredients usually presented as required for Darwinian evolution: heredity, variation and selection. A system that would possess the three while being coupled to some sort of encapsulated replication process would theoretically be able to undergo Darwinian evolution. As a matter of fact, this has been shown theoretically for Collectively Autocatalytic Sets (CAS) where each molecule of the set is catalytically formed by another member of the ensemble. Here we use the Azoarcus recombination ribozyme system to experimentally form structurally diverse CASs to explore their evolutionary properties. In this system, the ribozymes can catalyze the assembly of other ribozymes from smaller fragments, present in the food set. We first use a droplet microfluidics set-up coupled with next-generation sequencing to conduct a large scale study on thousands of Azoarcus CASs. We develop a perturbative approach to identify the important topological parameters that control variations in CASs as a result of environmental perturbations, here the addition of a new species. We then determine the small set of network features governing memory of the initial conditions in Azoarcus CAS, a pre-requisite for heredity, by using a computational model validated by experimental data. Finally, we demonstrate that Azoarcus CAS possess catabolic processes which make them robust to perturbations in the food set and thus more prebiotic relevant. These results provide evidence for the crucial role of RNA CASs in the origins of life and illustrate how the network structure can be tailored to obtain CASs with properties interesting from an evolutionary point of view, paving the way to an experimental demonstration of Darwinian evolution with a purely molecular system
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6

Eden-Jones, Kym Denys. "Kinetic Monte Carlo simulations of autocatalytic protein aggregation." Thesis, University of Edinburgh, 2014. http://hdl.handle.net/1842/9365.

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The self-assembly of proteins into filamentous structures underpins many aspects of biology, from dynamic cell scaffolding proteins such as actin, to the amyloid plaques responsible for a number of degenerative diseases. Typically, these self-assembly processes have been treated as nucleated, reversible polymerisation reactions, where dynamic fluctuations in a population of monomers eventually overcome an energy barrier, forming a stable aggregate that can then grow and shrink by the addition and loss of more protein from its ends. The nucleated, reversible polymerisation framework is very successful in describing a variety of protein systems such as the cell scaffolds actin and tubulin, and the aggregation of haemoglobin. Historically, amyloid fibrils were also thought to be described by this model, but measurements of their aggregation kinetics failed to match the model's predictions. Instead, recent work indicates that autocatalytic polymerisation - a process by which the number of growth competent species is increased through secondary nucleation, in proportion to the amount already present - is better at describing their formation. In this thesis, I will extend the predictions made in this mean-field, autocatalytic polymerisation model through use of kinetic Monte Carlo simulations. The ubiquitous sigmoid-like growth curve of amyloid fibril formation often possesses a notable quiescent lag phase which has been variously attributed to primary and secondary nucleation processes. Substantial variability in the length of this lag phase is often seen in replicate experimental growth curves, and naively may be attributed to fluctuations in one or both of these nucleation processes. By comparing analytic waiting-time distributions, to those produced by kinetic Monte Carlo simulation of the processes thought to be involved, I will demonstrate that this cannot be the case in sample volumes comparable with typical laboratory experiments. Experimentally, the length of the lag phase, or "lag time", is often found to scale with the total protein concentration, according to a power law with exponent γ. The models of nucleated polymerisation and autocatalytic polymerisation predict different values for this scaling exponent, and these are sometimes used to identify which of the models best describes a given protein system. I show that this approach is likely to result in a misidentification of the dominant mechanisms under conditions where the lag phase is dominated by a different process to the rest of the growth curve. Furthermore, I demonstrate that a change of the dominant mechanism associated with total protein concentration will produce "kinks" in the scaling of lag time with total protein concentration, and that these may be used to greater effect in identifying the dominant mechanisms from experimental kinetic data. Experimental data for bovine insulin aggregation, which is well described by the autocatalytic polymerisation model for low total protein concentrations, displays an intriguing departure from the predicted behaviour at higher protein concentrations. Additionally, the protein concentration at which the transition occurs, appears to be affected by the presence of salt. Coincident with this, an apparent change in the fibril structure indicates that different aggregation mechanisms may operate at different total protein concentrations. I demonstrate that a transition whereby the self-assembly mechanisms change once a critical concentration of fibrils or fibrillar protein is reached, can explain the observed behaviour and that this predicts a substantially higher abundance of shorter laments - which are thought to be pathogenic - at lower total protein concentrations than if self-assembly were consistently autocatalytic at all protein concentration. Amyloid-like loops have been observed in electron and atomic-force microscographs, together with non-looped fibrils, for a number of different proteins including ovalbumin. This implies that fibrils formed of these proteins are able to grow by fibrillar end-joining, and not only monomer addition as is more commonly assumed. I develop a simple analytic expression for polymerisation by monomer addition and fibrillar end-joining, (without autocatalysis) and show that this is not sufficient to explain the growth curves obtained experimentally for ovalbumin. I then demonstrate that the same data can be explained by combining fibrillar end-joining and fragmentation. Through the use of an analytic expression, I estimate the kinetic rates from the experimental growth curves and, via simulation, investigate the distribution of lament and loop lengths. Together, my findings demonstrate the relative importance of different molecular mechanisms in amyloid fibril formation, how these might be affected by various environmental parameters, and characteristic behaviour by which their involvement might be detected experimentally.
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7

Evans, Robert. "The effect of magnetic fields on autocatalytic chemical reactions." Thesis, University of Oxford, 2007. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.444929.

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8

Quaranta, Michela. "Mechanistic study of asymmetric amplification in the Soai autocatalytic reaction." Thesis, Imperial College London, 2010. http://hdl.handle.net/10044/1/6202.

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Soai’s discovery of chiral amplification in the autocatalytic alkylation of pyrimidine-5-carbaldehyde with diisopropylzinc is one of the most noteworthy findings of the last decade of the 20th century. This is the first experimental confirmation of an early theoretical rationalisation of autocatalysis as a mechanism for the evolution of biological homochirality from a racemic environment (Frank, 1953). This thesis describes kinetic and spectroscopic investigations that were conducted with the aim of better understanding the mechanism under which chiral amplification is achieved in the Soai system. The methodology used to perform the kinetic studies that are presented in this thesis focuses on the use of reaction calorimetry as in-situ tool coupled with the appropriate analytical technique for enantiomeric excess measurements. Observations of an unusual temperature effect on the reaction rate and a profound induction period are reported together with extensive kinetic investigations. Kinetic experiments were designed and carried out following Reaction Progress Kinetic Analysis methodology, which is described in detail. These experiments were carried out in order to ascertain the concentration dependence of the substrates and the reaction product, and revealed a 1.6 order in pyrimidyl aldehyde, a zero order in diisopropylzinc and a first order in the reaction product. Meticulous NMR studies of the alkoxide product at low temperature demonstrated its tendency to form tetrameric complexes, which could be either directly involved in the autocatalysis or be the precursors of the active catalytic species. Possible mechanisms that involve tetramers formation are proposed and supported by simulations carried out using COPASI simulation software. This thesis also includes a separate Chapter on the MIB mediated alkylation of benzaldehyde with diethylzinc, a system characterised by a marked nonlinear effect. Kinetic studies demonstrate how the high degree of chiral amplification comes at the expense of the reaction rate.
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9

Al-Mannai, Muna. "Finite-difference methods for some non-linear reaction-diffusion systems in chemistry." Thesis, Brunel University, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.390219.

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10

Baer, Brian R. "Autocatalytic mechanism and functional consequences of covalent heme attachment in CYP4B1 /." Thesis, Connect to this title online; UW restricted, 2005. http://hdl.handle.net/1773/8176.

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11

Sharma, Krishna. "Cation-controlled diastereo- and enantioselective synthesis of indolines : an autocatalytic process." Thesis, University of Oxford, 2014. http://ora.ox.ac.uk/objects/uuid:bfec8a97-7740-49f9-aa8f-5b97f632c21d.

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Asymmetric phase-transfer catalysis is a powerful technique that enables a wide range of transformations under mild conditions, often using inexpensive and environmentally benign reagents. By extending the applications of phase-transfer catalysis we have developed a highly diastereo- and enantioselective synthesis of functionalized indolines bearing two contiguous stereocentres, one of which is quaternary and all carbon, in a single synthetic step. The reaction proceeds with complete diastereoselectivity and with high levels of enantioselectivity (up to 99% ee). Despite the development of phase-transfer catalysis as a primary synthetic tool in organic synthesis, the mechanistic understanding of these reactions still remains a challenge, due mainly to the difficulty of studying the complex multi-phase systems. Therefore, a further aim of this project was to understand the reaction mechanism of our phase-transfer catalysed transformation. Investigations into the mechanism of our phase-transfer catalysed reaction have been carried out by studying the reaction kinetics. These have shown that the reaction follows a sigmoidal curve with an induction period present. A detailed kinetic investigation was carried out which demonstrated that an autocatalytic mechanism is operational.
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12

Fusion, Joe. "The Role of Environmental Dynamics in the Emergence of Autocatalytic Networks." PDXScholar, 2015. https://pdxscholar.library.pdx.edu/open_access_etds/2458.

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For life to arise from non-life, a metabolism must emerge and maintain itself, distinct from its environment. One line of research seeking to understand this emergence has focused on models of autocatalytic reaction networks (ARNs) and the conditions that allow them to approximate metabolic behavior. These models have identified reaction parameters from which a proto-metabolism might emerge given an adequate matter-energy flow through the system. This dissertation extends that research by answering the question: can dynamically structured interactions with the environment promote the emergence of ARNs? This question was inspired by theories that place the origin of life in contexts such as diurnal or tidal cycles. To answer it, an artificial chemistry system with ARN potential was implemented in the dissipative particle dynamics (DPD) modeling paradigm. Unlike differential equation (DE) models favored in prior ARN research, the DPD model is able to simulate environmental dynamics interacting with discrete particles, spatial heterogeneity, and rare events. This dissertation first presents a comparison of the DPD model to published DE results, showing qualitative similarity with some interesting differences. Multiple examples are then provided of dynamically changing flows from the environment that promote emergent ARNs more than constant flows. These include specific cycles of energy and mass flux that consistently increase metrics for ARN concentration and mass focusing. The results also demonstrate interesting nonlinear interactions between the system and cycle amplitude and period. These findings demonstrate the relevance that environmental dynamics has to ARN research and the potential for broader application as well.
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13

Mee, Trevor Richard. "Analysis of the proteolytic cleavage reaction of the tumour suppressor protein p53." Thesis, University of York, 1999. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.310987.

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14

Bárcena, Menéndez Diego 1984. "A study on autocatalysis through synthetic biology. Exploration of spatiotemporal dynamics in the presence or absence of synthetic autocatalytic Hepatocyte Growth Factor signaling in mammalian cells." Doctoral thesis, Universitat Pompeu Fabra, 2016. http://hdl.handle.net/10803/523520.

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Una de las preguntas sin resolver en la biologia celular, es como las células mamíferas logran generar patrones estables como organos o seres vivos, en un entorno variable. El concepto matemático del bucle de retreoalimentación, es una herramienta que puede generar orden. En esta tesis, presento dos proyectos que forman parte de una idea iterativa para recrear patrones biológicos sintéticamente en células mamíferas. En la primera parte, presento la creación de una linea celular que funge como detector de niveles de la hormona HGF a través de una reportero transcripcional. En la segunda parte, demuestro la reprogramación de esta células con fin de producir HGF en respuesta a HGF, en efecto creando un bucle de retroalimentación positivo. En ambos proyectos, utilizo microscopia cuantitativa espaciotemporal para analyzar y medir la evolución dinámica de las células en respuesta a un estímulo de HGF.
One unanswered riddle in biology is how can mammalian cells organize to generate ordered patterns such as organs and living beings, in an ever changing environment. An underlying mathematical principle for the generation of order is given by feedback motifs. Here, I present two projects which are part of an effort to recreate stable ordered patterns in a cellular system through information encoded in DNA. In the first part, I present a receiver mammalian cell line which can accurately sense the diffusible Hepatocyte Growth Factor (HGF) through a transcriptional reporter. In the second part I reprogrammed this cell line so that it produces more HGF in response to HGF, in effect creating an autocatalytic positive feedback. In both cases, I have used spatiotemporal quantitative microscopy analysis to monitor the dynamic evolution of the cell lines in response to a HGF stimulus.
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15

Mhatre, Bharat Suresh. "Super-enantiospecific Autocatalytic Decomposition of Tartaric Acid and Aspartic Acid on Cu Surfaces." Research Showcase @ CMU, 2013. http://repository.cmu.edu/dissertations/232.

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Autocatalytic reaction mechanisms are observed in a range of important chemical processes including catalysis, radical-mediated explosions, and biosynthesis. Because of their complexity, the microscopic details of autocatalytic reaction mechanisms have been difficult to study on surfaces and heterogeneous catalysts. Autocatalytic decomposition reactions of tartaric acid (TA) enantiomers adsorbed on Cu(110) offer molecular-level insight into these processes, which until now, were largely a matter of speculation. The decomposition of TA/Cu(110) is initiated by a slow, irreversible process that forms vacancies in the adsorbed TA layer, followed by a vacancy-mediated, explosive decomposition process that yields CO2 and small hydrocarbon products. Initiation of the explosive decomposition of TA/Cu(110) was studied by measurement of the reaction kinetics, time-resolved low energy electron diffraction (LEED), and time-resolved scanning tunneling microscopy (STM). Initiation results in a decrease in the local coverage of TA and a concomitant increase in the areal vacancy concentration. Once the vacancy concentration reaches a critical value, the explosive, autocatalytic decomposition step dominates the subsequent TA decomposition rate. Aspartic acid is an excellent probe molecule for investigating the surface chemistry of autocatalytic reactions . Because a wide range of isotopically labeled varieties of aspartic acid are commercially available, we have been able to conduct a detailed investigation of its autocatalytic reaction mechanism. Experimental data obtained for variable initial coverage, variable heating rate and isothermal TPRS experiments, while monitoring CO2 desorption is in excellent agreement with a rate law which explicitly accounts for an initiation step and an explosion step which is second order in vacancy concentration Autocatalytic surface explosion mechanisms can be exploited to attain extremely high enantiospecificities in the case of TA decomposition on naturally chiral Cu(hkl)R&S surfaces. Interaction energies of chiral molecules with naturally chiral surfaces are small and typically lead to modest enantioselectivities. However, the highly non-linear kinetics of autocatalytic reaction mechanism amplifies these small differences to result in high enantiospecificities. The observed phenomenon has the characteristics of autocatalytic processes that have been postulated to lead to biomolecular homochirality in life on Earth; processes with relatively small differences in reaction energetics that, nonetheless, lead to extremely high enantioselectivity.
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16

Glöde, Patric Karl [Verfasser], and Andreas [Akademischer Betreuer] Greven. "Dynamics of Genealogical Trees for Autocatalytic Branching Processes / Patric Karl Glöde. Betreuer: Andreas Greven." Erlangen : Universitätsbibliothek der Universität Erlangen-Nürnberg, 2013. http://d-nb.info/1033029912/34.

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17

Glöde, Patric [Verfasser], and Andreas [Akademischer Betreuer] Greven. "Dynamics of Genealogical Trees for Autocatalytic Branching Processes / Patric Karl Glöde. Betreuer: Andreas Greven." Erlangen : Universitätsbibliothek der Universität Erlangen-Nürnberg, 2013. http://nbn-resolving.de/urn:nbn:de:bvb:29-opus-45453.

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18

Blanken, Erika. "A NUMERICAL ANALYSIS APPROACH FOR ESTIMATING THE MINIMUM TRAVELING WAVE SPEED FOR AN AUTOCATALYTIC REACTION." Master's thesis, University of Central Florida, 2008. http://digital.library.ucf.edu/cdm/ref/collection/ETD/id/2389.

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This thesis studies the traveling wavefront created by the autocatalytic cubic chemical reaction A + 2B → 3B involving two chemical species A and B, where A is the reactant and B is the auto-catalyst. The diffusion coefficients for A and B are given by and . These coefficients differ as a result of the chemical species having different size and/or weight. Theoretical results show there exist bounds, and , depending on , where for speeds , a traveling wave solution exists, while for speeds , a solution does not exist. Moreover, if , and are similar to one another and in the order of when it is small. On the other hand, when there exists a minimum speed vmin, such that there is a traveling wave solution if the speed v > vmin. The determination of vmin is very important in determining the dynamics of general solutions. To fill in the gap of the theoretical study, we use numerical methods to determine vmin for various cases. The numerical algorithm used is the fourth-order Runge-Kutta method (RK4).
M.S.
Department of Mathematics
Sciences
Mathematical Science MS
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19

Eriksson, Mats. "Sliding wear performance of electroplated hard chromium and autocatalytic nickel-phosphorus coatings at elevated temperatures." Thesis, Karlstads universitet, Avdelningen för maskin- och materialteknik, 2014. http://urn.kb.se/resolve?urn=urn:nbn:se:kau:diva-34870.

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This thesis was written for a Swedish valve manufacturer to find out in what temperature regimes it was possible to replace electroplated hard chromium with autocatalytic electroless nickel-phosphorus. In this work the dry sliding wear properties of electroplated hard chromium and autocatalytic electroless nickel-phosphorus(10% P) were compared. All tests and investigations were done by using available equipment at Karlstads University. The tests were made to find out how the wear of these coatings behaved at different temperatures, how different substrates influence the wear of these coatings and how the roughness of the substrate surface influence the wear properties of these coatings. The method used for the wear tests was block-on-ring with a counterformal contact mode. The tests were executed in room temperature, 300C and 400C; with a normal load of 100N, sliding speed was 150rpm and duration of the tests were 15 minutes. All tests were done in an argon gas atmosphere. The coatings was deposited onto the cylinders with a thickness of 30µm. The different substrates used were an austenitic stainless steel(1.4404) and an austenitic-ferritic(duplex) stainless steel(1.4460). Half of the austenitic cylinders had a machined surface and all the others(including duplex cylinders) were machined and grinded to achieve a smoother surface. The blocks used as countersurface were made out of austenitic-ferritic(duplex) stainless steel(1.4460). Equipment used to investigate the wear tracks were stereo microscopy, profilometer, microhardness tester and scanning electron microscopy(SEM). The coatings were investigated in matter such as wear depth, wear mode, wear mechanism, chemical composition, topography, morphology, cross-section and hardness. The results of this work showed that the nickel coating wear tracks maximal depth were less deep than those of hard chrome, at room temperature. At elevated temperatures the performance varies. The coatings deposited onto cylinders made out of duplex stainless steel performed better than those deposited onto austenitic cylinders. The nickel coating performed better deposited onto the substrates with smooth surface and the chrome coating performed better deposited onto the substrates with rough surface
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20

Baumdick, Martin [Verfasser], Philippe [Akademischer Betreuer] Bastiaens, and Roger S. [Gutachter] Goody. "Dynamic regulation of autocatalytic EGFR activation / Martin Baumdick ; Gutachter: Roger S. Goody ; Betreuer: Philippe Bastiaens." Dortmund : Universitätsbibliothek Dortmund, 2017. http://d-nb.info/1160443157/34.

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21

Iwamura, Hiroshi. "Mechanistic insights from kinetic analysis by reaction calorimetry into proline-catalyzed asymmetric reactions and autocatalytic reaction." 京都大学 (Kyoto University), 2006. http://hdl.handle.net/2433/136952.

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22

Prušinskas, Kęstutis. "Investigation of the autocatalytic Cu(II) reduction processes in the systems with natural polyhydroxylic compounds as ligands." Doctoral thesis, Lithuanian Academic Libraries Network (LABT), 2013. http://vddb.laba.lt/obj/LT-eLABa-0001:E.02~2013~D_20130114_082011-57496.

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This work investigates polyols – glycerol and sucrose – as an alternative ligand for electroless copper plating systems with reducer formaldehyde. Natural polyols are environmentally friendly, easily bio-degradable materials, but has not been studied enough for suitability for copper plating systems. In order to increase of the efficiency, the electroless copper plating was investigated in ultrasonic milieu to observe how ultrasound impacts the copper plating rate and properties of the obtained coatings. Studies have shown that sucrose and glycerol can be used as ligands in solutions for electroless copper plating. A plating rate of copper under optimum conditions can reach 2.2 m h-1 (sucrose) and 3.4 m h-1 (glycerol) and copper surface roughness factors ranging 8.5 - 25.3 (sucrose) and 2,3 - 4.3 (glycerol). Correlations between dependences on pH observed for copper plating speeds, overpotentials, surface roughness factors, anodic oxidation currents of formaldehyde. A use of ultrasound for electroless copper plating systems change speeds. Depending on the choice of copper plating system and ultrasonic frequency, plating rate can decrease or may increase up to 5 times and can reach high values (10.87 m h-1). The copper surface formed in ultrasound environment more compact, smoother.
Šiame darbe tiriami polihidroksiliai alkoholiai sacharozė bei glicerolis, kaip ligandų alternatyvos cheminio variavimo sistemoms su reduktoriumi formaldehidu. Tai yra ekologiškos, biologiškai lengvai suyrančios medžiagos. Šiame darbe atlikti šių medžiagų kompleksų pusiausvyros skaičiavimai, eksperimentai parodantys sacharozės bei glicerolio praktinį pritaikomumą cheminio variavimo sistemose. Ultragarso poveikio cheminėms sistemoms dėsningumai dar nėra vienareikšmiškai ištirti ir suprasti. Siekiant padaryti cheminį metalų nusodinimą efektyvesniu pastaruoju metu cheminio metalizavimo procesams bandoma taikyti ultragarsą. Atlikti tyrimai parodė, kad naudojant sacharozę ir glicerolį ligandais cheminio variavimo tirpaluose vario nusėdimo greitis optimaliomis sąlygomis siekia atitinkamai 2,2 ir 3,4 m/h, o chemiškai nusodinto vario paviršiaus šiurkštumo faktoriai varijuoja 8,5-25,3 ir 2,3-4,3 ribose. Analizuojant gautus duomenis stebimos koreliacijos tarp vario nusėdimo greičio, viršįtampio, paviršiaus šiurkštumo faktoriaus, formaldehido anodinės oksidacijos srovių maksimumų priklausomybių nuo pH. Ultragarso panaudojimas cheminio variavimo sistemose keičia vario nusėdimo greičius. Priklausomai nuo pasirinktos cheminio variavimo sistemos, ultragarso dažnio ar jo skleidimo būdo vario nusėdimo greitis sumažėja iki visiško proceso sustabdymo arba gali padidėti 2-5 kartus ir pasiekti dideles vertes (10,87 μm/h). Ultragarso aplinkoje dažniausiai susiformuoja kompaktiškesnės, lygesnės... [toliau žr. visą tekstą]
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23

Gardner, Bryan (Bryan Jay). "Lean Transformations in Supply Chain, the autocatalytic nature of lean principles, and tactics for implementing lean tools." Thesis, Massachusetts Institute of Technology, 2008. http://hdl.handle.net/1721.1/43834.

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Thesis (M.B.A.)--Massachusetts Institute of Technology, Sloan School of Management; and, (S.M.)--Massachusetts Institute of Technology, Dept. of Aeronautics and Astronautics; in conjunction with the Leaders for Manufacturing Program at MIT, 2008.
Includes bibliographical references (p. 179).
Expanding Lean principles beyond the manufacturing floor, ultimately to entail a comprehensive Lean Enterprise, has gained increasing attention among corporations. This thesis entails a detailed case study of initiating a Lean Transformation in the Supply Chain department of a technology center for engineering, integration and final assembly of directional drilling equipment. This technology center is part of Schlumberger, a global corporation and industry leader in directional drilling and other oilfield technologies and services. Initiating the Lean Transformation in this Supply Chain department is detailed and used as the central theme throughout the thesis. The rapid, successive applications and results of conventional Lean principles are evaluated. Due to the near relative proximity of the several initiatives undertaken, in both time and within the organization, this case is used to evaluate the Autocatalytic Nature of Lean Principles within the Supply Chain department. Concurrently, the dynamics involved with the interactions of personnel within the department are evaluated. As a Lean Transformation is so heavily dependent upon the personnel participating in the change, tactics for initiating a Lean Transformation are treated in reference to the several initiatives of this case study. These three components, Lean principles, their autocatalytic interaction, and relevant human interactions, are all combined to comprehensively address the most influential aspects of affecting a Lean Transformation in a Supply Chain department.
by Bryan Gardner.
S.M.
M.B.A.
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24

Miu, Kevin (Kevin K. ). "The development of autocatalytic structural materials for use in the sulfur-iodine process for the production of hydrogen." Thesis, Massachusetts Institute of Technology, 2006. http://hdl.handle.net/1721.1/36724.

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Thesis (S.B.)--Massachusetts Institute of Technology, Dept. of Mechanical Engineering; and, (S.B.)--Massachusetts Institute of Technology, Dept. of Nuclear Engineering, 2006.
Includes bibliographical references (p. 63).
The Sulfur-Iodine Cycle for the thermochemical production of hydrogen offers many benefits to traditional methods of hydrogen production. As opposed to steam methane reforming - the most prevalent method of hydrogen production today - there are no carbon dioxide emissions. Compared to other methods of hydrogen production, the efficiency of the cycle is excellent. Due to the high temperatures necessary for the cycle, which are generally greater than 8500C, several of the Generation IV nuclear reactor concepts are attractive thermal energy sources. However, the high temperature and corrosive reaction conditions of the cycle, involving reactions including the decomposition of H2SO4 at 400-9000C, present formidable corrosion challenges. The conversion of sulfuric acid to sulfur dioxide was the focus of this study. The alloying of structural materials to platinum has been proposed as a solution to this problem. A catalytic loop to test the materials was constructed. Sulfuric acid was pumped over the material at 903+20C. The sulfur dioxide production of the catalyst was measured as a means of quantifying the efficiency of the system as a function of temperature.
(cont.) The maximum possible production of the material was calculated by using a mass balance. A gas chromatograph was used to calculate the actual production of sulfur dioxide. The results of the experiment show that an molecular conversion efficiency of 10% is attained when operating at 900C while using 800H + 5%Pt as a catalyst. The research confirms the catalytic activity of the material.
by Kevin Miu.
S.B.
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25

Boerner, Susann. "Probing reaction conditions and cofactors of conformational prion protein changes underlying the autocatalytic self-propagation of different prion strains." Doctoral thesis, Humboldt-Universität zu Berlin, Lebenswissenschaftliche Fakultät, 2014. http://dx.doi.org/10.18452/17003.

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Prionen sind das infektiöse Agens transmissibler spongiformer Enzephalopathien von Tieren und Menschen. Prionen bestehen hauptsächlich aus einer abnormal gefalteten und aggregierten Isoform des zellulären Prionproteins (PrP). Die Replikation von Prionen findet mutmaßlich durch keiminduzierte Polymerisation des Prionproteins statt. Es existieren verschiedene Prionstämme, die unterschiedliche Eigenschaften aufweisen, aber vom selben zellulären Prionprotein abstammen können. Neben PrP scheinen Kofaktormoleküle an der Prionreplikation beteiligt zu sein. Weiterhin wird angenommen, dass Kofaktoren bei der Definition von Stammeigenschaften beteiligt sind, sowie ein Einfluss auf die Infektiosität von Prionen besteht. In dieser Arbeit wurden die Auswirkungen verschiedener Kofaktoren auf die Replikation von vier Hamster-adaptierten Prionstämmen in vitro mittels der Methode der „Protein Misfolding Cyclic Amplification“ (PMCA) untersucht. Es wurden stammabhängige Unterschiede bezüglich der Anforderungen an die Replikationsbedingungen in der PMCA, sowie Kofaktor-Selektivitäten festgestellt. Der Einfluss von Kofaktoren wurde durch den Vergleich ausgewählter biologischer, biochemischer und biophysikalischer Eigenschaften von in vitro erzeugten PMCA Produkten (PrPres) mit denen nativer Prionkeime untersucht. Es zeigte sich, dass Kofaktoren Stammeigenschaften, wie die biologische Keimaktivität in primären Gliazellkulturen und biochemische Eigenschaften, wie die Migration in SDS-Gelen, beeinflussen können. Um festzustellen, ob unterschiedliche Kofaktorbedingungen während der PMCA messbare Veränderungen der Proteinkonformation hervorrufen, wurde PMCA generiertes PrPres mittels FT-IR Spektroskopie in einer Pilotstudie charakterisiert. Erste Befunde zeigten spektrale Unterschiede zwischen den Proteinkeimen und deren PMCA Produkten bei allen Stämmen, unabhängig von den Kofaktorbedingungen.
Prions are the causative agent of transmissible spongiform encephalopathies in animals and humans such as scrapie, bovine spongiform encephalopathy (BSE) and Creutzfeldt-Jakob disease (CJD). Prions are thought to be composed essentially of a misfolded and aberrantly aggregated isoform of the cellular prion protein (PrP) and to replicate by seeded PrP polymerization. Prions may exist in the form of distinct strains that differ in their phenotypic characteristics although they are derived from the same cellular prion protein. Cofactor molecules other than PrP may be involved in prion replication and may be a determinant of strain properties. Furthermore, cofactors may also be required for conveying infectivity. The present study examined the effects of different cofactor molecules on the replication efficacy of four hamster adapted prion agents using the method of serial protein misfolding cyclic amplification (PMCA) as in vitro assay for PrP misfolding and aggregation. The study revealed strain dependent differences of PMCA conditions and cofactors required for efficient in vitro replication. The impact of cofactors was assessed by comparative analyses of selected biological, biochemical and biophysical properties of PMCA products (PrPres) and native prion seeds. The biological seeding activity as monitored in a primary hamster glial cell assay, and biochemical properties such as electrophoretic migration in SDS-gels, were affected differently by different cofactors. In order to define the impact of putative cofactors on the molecular conversion of PrP in more detail, changes in the spatial structure associated with different cofactor molecule conditions during amplification of PrPres in PMCA was monitored by Fourier transform-infrared (FT-IR) spectroscopic analysis. Largely preliminary data revealed spectral differences between native prion seeds and progeny PMCA generated PrPres for all prion strains, but no variations due to different cofactor conditions.
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26

Chakraborty, Aryadeep Verfasser], Hans-Josef [Akademischer Betreuer] Allelein, Nabiha [Akademischer Betreuer] Chaumeix, and Heinz Günter [Akademischer Betreuer] [Pitsch. "Optimization of passive autocatalytic recombiners (PARs) with respect to gas-phase ignition / Aryadeep Chakraborty ; Hans-Josef Allelein, Nabiha Chaumeix, Heinz Pitsch." Aachen : Universitätsbibliothek der RWTH Aachen, 2020. http://d-nb.info/1225401674/34.

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27

Gencer, Burcak. "Analysis Of Self-processing Mechanism Of Galactose Oxidase By Site-directed Mutagenesis And Heterologous Expression In Escherichia Coli." Master's thesis, METU, 2005. http://etd.lib.metu.edu.tr/upload/3/12607081/index.pdf.

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In this study, self-catalytic maturation of heterologously expressed pro-galactose oxidase was analysed in E.coli by altering some amino acids which were supposed to play a crucial role in pro-peptide removal. Galactose oxidase (GOase
EC 1.1.3.9) from Fusarium graminearum
having a molecular mass of 68kDa, is a monomeric, copper containing enzyme with an unusual thioether bond. The enzyme is produced as a precursor with an additional 8 amino acid pre- and a 17- amino acid pro-sequence at the N terminus. Previous work has shown that the pre-peptide is removed possibly by a protease during secretion, whereas the 17 amino acid pro-peptide is removed autocatalytically by the aerobic addition of Cu2+ to the precursor, preceding the formation of the thioether bond at the active site. The pro-gao gene was on ProGON1 and ProGOMN1 constructs which were previously established on pET101/D/lacZ vector in England by directed evolution. ProGON1 contains silent mutations at the N-terminus different from native galactose oxidase whereas ProGOMN1 has six further mutations within the mature enzyme, providing high expression. The cleavage site mutations R-1P/A1P, R-1X/A1X, S2A, and the H522A mutation just against the cleavage site in the three dimensional configuration, were carried out by site-directed mutagenesis. Those and some extra mutations were confirmed by DNA sequence analysis. Next, mutant galactose oxidases were expressed in E. coli BL21 Star (DE3), and were purified by Strep-Tactin®
Sepharose®
column, operating on the basis of affinity chromatography. Subsequently, SDS-PAGE was performed to analyze self-processing by detecting molecular mass difference of protein bands resulting from pro-sequence removal or existence. When the bands obtained in SDS-PAGE were compared, it was seen that the products of original recombinant plasmids, i.e. ProGON1, ProGOMN1
and the mutational variants showed no difference in band size, all slightly above 70kDa
indicating pro-sequence presence on all constructs. Non-mutants and some of the mutants showed galactose oxidase activity, signifying proper active site construction by thioether bond formation. ProGOMN1 was submitted for N-terminal amino acid sequencing to be able to assert that a size above 70kDa is not solely due to the existence of a 1 kDa Strep-tag II at C-terminus. Sequencing data affirmed the presence of both the pre-peptide and the pro-preptide showing that processing has not occurred at the N-terminus. Accordingly, in this study, it was shown for the first time that the existence of a pre-pro-peptide at the N-terminus of galactose oxidase does not prevent thioether bond formation at the active site. Furthermore, since the pro-peptide is cleaved autocatalytically, the lack of removal of the pre-peptide in E.coli in the presence of Cu 2+ and oxygen is very likely to be the cause of lack of pro-peptide cleavage. In future studies the region corresponding to the pre-peptide will be deleted to prove this hypothesis.
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28

Cardoso, Cristiano. "Revestimentos de níquel químico para proteção contra corrosão." Universidade de São Paulo, 2006. http://www.teses.usp.br/teses/disponiveis/3/3133/tde-11122006-132846/.

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O revestimento de níquel químico é largamente utilizado na proteção contra a corrosão de equipamentos e estruturas utilizados na exploração de petróleo em águas profundas. Apesar de ser considerado um dos revestimentos mais adequados para esta finalidade, são muitos os casos em que se verificam falhas prematuras do revestimento em serviço. Isto tem sido atribuído às diferenças nas características do revestimento decorrentes das diferenças do processo de aplicação e da natureza e preparação da superfície dos substratos a serem protegidos. Estas diferenças decorrem do fato de não existirem especificações abrangentes que definam as características necessárias do revestimento para uma garantia de qualidade. Diante disto, o presente trabalho teve como objetivo estudar a influência dos principais fatores sobre o desempenho dos revestimentos de níquel químico utilizando ferramentas estatísticas como: planejamento fatorial, seleção dos melhores subconjuntos de regressão, regressão múltipla e curvas de nível. Os fatores considerados neste estudo foram: tipo e estado superficial do substrato, idade do banho, teor de fósforo no revestimento, natureza e teor de contaminantes no revestimento, espessura do revestimento e tipo de tratamento térmico. A caracterização dos revestimentos de níquel químico foi realizada conforme sugerida na norma ISO 4527 e o desempenho dos revestimentos foi verificado por meio dos ensaios de exposição à névoa salina (1 536 h), exposição ao dióxido de enxofre (10 ciclos) e imersão em água do mar sintética (120 dias). Ensaios eletroquímicos (polarização linear e espectroscopia de impedância eletroquímica) foram realizados somente com o intuito de compará-los ao ensaio de exposição à névoa salina e,assim, ter um ensaio capaz de verificar revestimentos de bom desempenho em um período de tempo menor. Dentro dos intervalos estudados, verificou-se que o desempenho do revestimento de níquel químico é influenciado pelo tipo de substrato, pela espessura da camada depositada, pelo teor de fósforo, pela idade do banho, pelo tratamento térmico e pelos teores dos seguintes contaminantes: enxofre, chumbo, magnésio, cobre, ferro e manganês. A metodologia estatística adotada permitiu verificar a interação entre os fatores influenciadores, fato não considerado na literatura consultada. Além disto, foi possível constatar que os ensaios adotados nas normas internacionais atuais são adequados para verificar a qualidade dos revestimentos. Verificou-se também que os ensaios eletroquímicos, apesar de adequados para o estudo da resistência intrínseca à corrosão do revestimento de níquel químico, não se mostraram adequados para detectar a presença de porosidade que é o principal indicativo da qualidade de proteção por barreira de revestimentos catódicos como o níquel químico. Com os resultados obtidos, será possível a elaboração de uma especificação para se obter revestimentos de níquel químico com bom desempenho.
The autocatalytic nickel-phosphorus (NiP) or electroless nickel (EN) coatings are widely used to protect equipment and structures against corrosion and erosion, used in the exploitation of petroleum in deep waters. Even though NiP is considered as the most appropriate coating for this purpose, many premature failures are verified in service. This has been attributed to the differences in the characteristics of the coating due to the differences in the application processes and in the nature and preparation of the substrate surfaces. The lack of broad specifications that define the required characteristics of the good quality coating is responsible for those differences. The present work had as its objective to identify the main factors related to the NiP performance using statistical tools as: factorial design, best subset regression, multiple regression and contour diagram. The considered factors were: substrate type, substrate surface finishing, bath age, phosphorus content, thickness, heat treatment and impurities. The NiP coatings were characterized in agreement with the ISO 4527 and their performance was verified through the salt spray test (1 536 h), the Kesternish test (10 cycles) and the synthetic sea water immersion test (120 days). Electrochemical tests (linear polarization and electrochemical impedance spectroscopy) were conducted in order to compare them to the salt spray test and thus reducing the testing time. In the studied range, it was verified that the NiP performance is influenced by the following factors: substrate type, thickness coating, phosphorus content, bath age (MTO), heat treatment and the impurities: sulfur, lead, magnesium, copper, iron and manganese. It was possible to verify that the types of accelerated corrosion tests adopted in the current international standards are appropriate to verify the quality of the coatings. It was also verified that the electrochemical tests, despite being suitable to indicate the NiP intrinsic corrosion resistance, are not appropriate to verify the NiP porosity (which is the main indication of a cathodic coating quality). With the obtained results, it will be possible to establish a better specification in order to obtain NiP with good quality.
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29

Gérard, Thomas. "Theoretical study of spatiotemporal dynamics resulting from reaction-diffusion-convection processes." Doctoral thesis, Universite Libre de Bruxelles, 2011. http://hdl.handle.net/2013/ULB-DIPOT:oai:dipot.ulb.ac.be:2013/209861.

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Dans les réacteurs industriels ou dans la nature, l'écoulement de fluides peut être couplé à des réactions chimiques. Dans de nombreux cas, il en résulte l'apparition de structures complexes dont les propriétés dépendent entre autres de la géométrie du système.

Dans ce contexte, le but de notre thèse a été d'étudier de manière théorique et sur des modèles réaction-diffusion-convection simples les propriétés de dynamiques spatio-temporelles résultant du couplage chimie-hydrodynamique.

Nous nous sommes focalisés sur les instabilités hydrodynamiques de digitation visqueuse et de densité qui apparaissent respectivement lorsqu'un fluide dense est placé au-dessus d'un fluide moins dense dans le champ de gravité et lorsqu'un fluide visqueux est déplacé par un fluide moins visqueux dans un milieu poreux.

En particulier, nous avons étudié les problèmes suivants:

- L'influence d'une réaction chimique de type A + B → C sur la digitation visqueuse. Nous avons montré que les structures formées lors de cette instabilité varient selon que le réactif A est injecté dans le réactif B ou vice-versa si ces réactifs n'ont pas un coefficient de diffusion ou une concentration initiale identiques.

- Le rôle de pertes de chaleur par les parois du réacteur dans le cadre de la digitation de densité de fronts autocatalytiques exothermiques. Nous avons caractérisé les conditions de stabilité de fronts en fonction des pertes de chaleur et expliqué l'apparition de zones anormalement chaudes lors de cette instabilité.

- L'influence de l'inhomogénéité du milieu sur la digitation de densité de solutions réactives ou non. Nous avons montré que les variations spatiales de perméabilité d'un milieu poreux peuvent figer ou faire osciller la structure de digitation dans certaines conditions.

- L'influence d'un champ électrique transverse sur l'instabilité diffusive et la digitation de densité de fronts autocatalytiques. Il a été montré que cette interaction peut donner lieu à des nouvelles structures et changer les propriétés du front.

En conclusion, nous avons montré que le couplage entre réactions chimiques et mouvements hydrodynamiques est capable de générer de nouvelles structures spatio-temporelles dont les propriétés dépendent entre autres des conditions imposées au système.

/

In industrial reactors or in nature, fluid flows can be coupled to chemical reactions. In many cases, the result is the emergence of complex structures whose properties depend among others on the geometry of the system.

In this context, the purpose of our thesis was to study theoretically using simple models of reaction-diffusion-convection, the properties of dynamics resulting from the coupling between chemistry and hydrodynamics.

We focused on the hydrodynamic instabilities of viscous and density fingering that occur respectively when a dense fluid is placed above a less dense one in the gravity field and when a viscous fluid is displaced by a less viscous fluid in a porous medium.

In particular, we studied the following issues:

- The influence of a chemical reaction type A + B → C on viscous fingering. We have shown that the fingering patterns observed during this instability depends on whether the reactant A is injected into the reactant B or vice versa if they do not have identical diffusion coefficients or initial concentrations.

- The role of heat losses through the reactor walls on the density fingering of exothermic autocatalytic fronts. We have characterized the conditions of stability of fronts depending on heat losses and explained the appearance of unusually hot areas during this instability.

- The influence of the inhomogeneity of the medium on the density fingering of reactive solutions or not. We have shown that spatial variations of permeability of a porous medium may freeze or generate oscillating fingering pattern under certain conditions.

- The influence of a transverse electric field on the Rayleigh-Taylor and diffusive instabilities of autocatalytic fronts. It was shown that this interaction may lead to new structures and may change the properties of the front.

In conclusion, we showed that the coupling between chemical reactions and hydrodynamic motions can generate new space-time structures whose properties depend among others, on the conditions imposed on the system.
Doctorat en Sciences
info:eu-repo/semantics/nonPublished

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30

Boerner, Susann [Verfasser], Erwin [Akademischer Betreuer] Schneider, Michael [Akademischer Betreuer] Beekes, and Walter J. [Akademischer Betreuer] Schulz-Schaeffer. "Probing reaction conditions and cofactors of conformational prion protein changes underlying the autocatalytic self-propagation of different prion strains / Susann Boerner. Gutachter: Erwin Schneider ; Michael Beekes ; Walter J. Schulz-Schaeffer." Berlin : Lebenswissenschaftliche Fakultät, 2014. http://d-nb.info/1054728364/34.

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31

Palmieri, Elena [Verfasser], Günter von [Gutachter] Kiedrowski, and Sijbren [Gutachter] Otto. "Autocatalytic desymmetrization of prochiral compounds : strategies to dictate and control self-replication in peptidic dynamic combinatorial libraries / Elena Palmieri ; Gutachter: Günter von Kiedrowski, Sijbren Otto ; Fakultät für Chemie und Biochemie." Bochum : Ruhr-Universität Bochum, 2018. http://d-nb.info/1154307719/34.

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32

Menon, Shakti Narayana. "Bifurcation problems in chaotically stirred reaction-diffusion systems." Thesis, The University of Sydney, 2008. http://hdl.handle.net/2123/3685.

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A detailed theoretical and numerical investigation of the behaviour of reactive systems under the influence of chaotic stirring is presented. These systems exhibit stationary solutions arising from the balance between chaotic advection and diffusion. Excessive stirring of such systems results in the termination of the reaction via a saddle-node bifurcation. The solution behaviour of these systems is analytically described using a recently developed nonperturbative, non-asymptotic variational method. This method involves fitting appropriate parameterised test functions to the solution, and also allows us to describe the bifurcations of these systems. This method is tested against numerical results obtained using a reduced one-dimensional reaction-advection-diffusion model. Four one- and two-component reactive systems with multiple homogeneous steady-states are analysed, namely autocatalytic, bistable, excitable and combustion systems. In addition to the generic stirring-induced saddle-node bifurcation, a rich and complex bifurcation scenario is observed in the excitable system. This includes a previously unreported region of bistability characterised by a hysteresis loop, a supercritical Hopf bifurcation and a saddle-node bifurcation arising from propagation failure. Results obtained with the nonperturbative method provide a good description of the bifurcations and solution behaviour in the various regimes of these chaotically stirred reaction-diffusion systems.
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33

Menon, Shakti Narayana. "Bifurcation problems in chaotically stirred reaction-diffusion systems." University of Sydney, 2008. http://hdl.handle.net/2123/3685.

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Doctor of Philosophy
A detailed theoretical and numerical investigation of the behaviour of reactive systems under the influence of chaotic stirring is presented. These systems exhibit stationary solutions arising from the balance between chaotic advection and diffusion. Excessive stirring of such systems results in the termination of the reaction via a saddle-node bifurcation. The solution behaviour of these systems is analytically described using a recently developed nonperturbative, non-asymptotic variational method. This method involves fitting appropriate parameterised test functions to the solution, and also allows us to describe the bifurcations of these systems. This method is tested against numerical results obtained using a reduced one-dimensional reaction-advection-diffusion model. Four one- and two-component reactive systems with multiple homogeneous steady-states are analysed, namely autocatalytic, bistable, excitable and combustion systems. In addition to the generic stirring-induced saddle-node bifurcation, a rich and complex bifurcation scenario is observed in the excitable system. This includes a previously unreported region of bistability characterised by a hysteresis loop, a supercritical Hopf bifurcation and a saddle-node bifurcation arising from propagation failure. Results obtained with the nonperturbative method provide a good description of the bifurcations and solution behaviour in the various regimes of these chaotically stirred reaction-diffusion systems.
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34

Burgess, D. J. "Autocatalysis in tributyl phosphate hydrolysis." Thesis, Swansea University, 1995. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.636178.

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The object of this study was to determine the kinetics and mechanism of the autocatalytic hydrolysis of tri-n-butylphosphate (TBP) in a hydrocarbon diluent (odourless kerosene (OK) or n-dodecane) by concentrated aqueous sodium hydroxide, typically 8.5 mol.dm-3. The reaction products are sodium dibutylphosphate (NaDBP) and butanol. Specific attention was paid to the formation of a third liquid phase during the reaction, the induction and autocatalytic periods of the reaction, and the importance of sodium hydroxide concentration. The induction period is shown to be the result of a homogeneous hydrolysis in the aqueous phase prior to third phase formation and the relevant second order homogeneous rate constants are determined. The NaDBP formed during this period is shown to be solubilised in both the organic and aqueous phases, the solubility of NaDBP in the TBP/diluent phase having a marked dependence on the phase composition. This dependence is speculated to be due to the formation of inverse micelles of NaDBP. Once these two phases are saturated with NaDBP the third phase is formed and autocatalysis begins. At low hydroxide concentrations no third phase is formed, all the NaDBP formed being solubilised in the aqueous phase and therefore no autocatalysis is observed. It is shown that the formation of the third phase eliminates the induction period and provides a homogeneous reaction solvent in which both reactants dissolve, the reaction being first order in both hydroxide ion and TBP, the second order homogeneous rate constants being determined. A simplistic kinetic model for the autocatalytic period of the reaction is presented and used in a computer simulation. The agreement between the simulated and experimentally observed data is discussed. NMR analysis is used to study the change in middle phase composition during the reaction. Further NMR studies on samples provided from the industrial process currently being used show that after six hours significant amounts of secondary hydrolysis occur forming sodium monobutylphosphate (Na2MBP).
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35

Kust, Paul Roger. "Micellar autocatalysis and mixed michelle thermodynamics." The Ohio State University, 1997. http://rave.ohiolink.edu/etdc/view?acc_num=osu1302028057.

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36

Kust, Paul Roger. "Micellar autocatalysis and mixed micelle thermodynamics /." The Ohio State University, 1997. http://rave.ohiolink.edu/etdc/view?acc_num=osu1487945015616522.

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37

Beauvier, Edouard. "Propagation d'un front de réaction-diffusion dans un écoulement cellulaire multi-échelle." Thesis, Aix-Marseille, 2013. http://www.theses.fr/2013AIXM4728/document.

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La propagation d'un front de réaction-diffusion est étudiée expérimentalement dans un écoulement cellulaire multiéchelle. Le front est produit par réaction autocatalytique en solution. L'écoulement est réalisé en géométrie de Hele-Shaw par électroconvection, son caractère multiéchelle étant réalisé par l'action combinée de deux nappes d'aimants d'échelles différentes. La géométrie du front et sa vitesse moyenne de propagation sont déterminées pour une large gamme d'intensité des vortex de chaque échelle. Elles sont confortées par une simulation numérique de l'avancée du domaine brulé dans le domaine frais. L'effet de la nature multiéchelle de l'écoulement sur la vitesse moyenne du front est compris par une méthode de renormalisation dont la validation est fournie par l'obtention d'un courbe maitresse pour l'ensemble des données
The propagation of a reaction-diffusion front is experimentally studied in a multi-scale cellular flow. The front is produced by an autocatalytic chemical reaction in an aqueous solution. The flow is generated by electroconvection and its multi-scale nature is induced by overlaying magnets of different scales. This enables an independent tune of the flow intensity at each scale. The geometry and the mean velocity of the front have been determined over a large range of scale intensities. These features are confirmed by a numerical simulation based on a burnt and fresh domain dynamics, the burnt domain expanding across the fresh one. The effect of the multi-scale nature of the flow on the mean front velocity is recovered by a renormalisation method validated by a collapse of the data onto a single curve
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38

Clairmont, Ryan Michael. "Azolium ions: A versatile framework for chemistry on early earth." Diss., Georgia Institute of Technology, 2016. http://hdl.handle.net/1853/55021.

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This work examines azolium catalysis of the small molecules formaldehyde and glyoxylic acid to yield product sugars as the starting point for synthesis of new azolium catalysts. It is broken into two projects: the first focusing on developing a proof of concept process to couple the two reactions, and the second expanding the reaction space using different solvents and catalyst. From these projects, a model for chemical evolution of small molecule catalysts was proposed. Reaction stoichiometry suggests that the process displays autocatalysis; however, the reactions were conducted separately so that kinetic enhancement was not observed. Even without kinetic enhancement, the findings indicate that synthesis of new catalyst from formaldehyde as the sole carbon source is possible, and that the process is robust due to effects such as catalyst deactivation or other loss pathways over time. Alternative work using glyoxylic acid demonstrated that the kinetics for carbohydrate synthesis are much slower.
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39

Billingham, John. "Travelling waves and clock reactions in quadratic and cubic autocatalysis." Thesis, University of East Anglia, 1991. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.280446.

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40

McGarry, John Kevin. "Application of bifurcation theory to physical problems." Thesis, University of Leeds, 1990. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.252925.

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41

McCabe, Philip M. "The mathematical analysis of a class of singular reaction-diffusion systems." Thesis, University of Reading, 1999. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.301978.

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42

Subramaniam, C. "Chemorhelogical Modeling Of Amine-Cured Multifunctional Epoxy Resin Systems Used As Matrices In Aerospace Composites." Thesis, Indian Institute of Science, 1994. http://hdl.handle.net/2005/127.

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High performance multifunctional epoxy resin systems are becoming increasingly important as matrix materials for the advanced composites used in aerospace, electronics, automotive and other industries. In a composite based on epoxy resin systems, a three-dimensional network of the matrix is formed around the reinforcing fibre as a result of the chemical reaction between the resin and the curing agent. This chemical process, known as curing, is an important event to he considered in the production of composite components made up of these resin systems. Two process parameters namely viscosity and chemical conversion are of paramount significance in the production of composite materials Curing studies of the resin systems based on these two parameters, would therefore assume great importance in deciding the performance reliability of the end product. The objectives of the present investigation are 1. to study the cure kinetics of three thermoset resin systems, viz., i) epoxy novolac (EPIT)/ diamino diphenyl methane{DDM), ii) trigylcidyl para- ammo phenol (TGPAP)/toluene diamine (TDA) and iii) tetraglycidyl diamino diphenyl methane (TGDDM)/pyridine diamine(PDA) using the cure kinetic models based on chemical conversion (α), Theological conversion (β) and viscosity. 2.to develop a correlation between a and viscosity (η) and modify an existing autocatalytic model based on α, to the viscosity domain and 3.to investigate the cure behaviour of these systems in terms of the TTT cure diagram and its associated models. EPN/DDM, TGPAP/PDA and TGDDM/PDA resin systems were chosen for the studies to represent a range of functionalities, The cure was monitored using differential scanning calorimetry (DSC), fourier transform infrared (FTIR) and dynamic mechanical analysis (DMA) techniques by following the changes in enthalpy, functional groups and rheology, respectively. The kinetic parameters namely, order of reaction and activation energy were estimated from dynamic DSC data using the methods of Freeman-Carroll and Ellerstein using nth rate expression. Barton, Kissinger and Osawa methods were employed to find out the activation energy from the peak/equal conversion at different heating rates. Isothermal DSC data were also analyzed using nth order model and it was observed that the data could be fitted satisfactorily only for higher temperatures The results obtained from the analysis of both dynamic and isothermal DSC data using nth order model clearly indicate that this model is inadequate for describing the cure behavior. The isothermal DSC data was analyzed by the autocatalytic models of Hone and Kamal Good correlation was observed with Hum and Kamal models up to 60-70%, 25% and 45% conversions for EPN/DDM, TGPAP/TDA and TCDDM/PDA systems respectively. However, the parameters m and n in Kamal model were found to be temperature dependent for EPN/DDM and TCPAP/TDA systems. The limited applicability of the autocatalytic models IK attributed to the counter-effect offered by the intra-molecular bonding taking place. The primary amine and epoxy groups conversions obtained from FTIR were analyzed using autocatalytic model and the kinetic parameters were calculated. The reactivity ratio of the primary amine and the secondary amine with epoxy was found to be dependent on temperature in agreement with the recent findings reported m the literature. The existing models that relate the cure kinetics and the rheological changes, are dual Arrhenius nth order model and autocatalytic model The nth order kinetic model was used to evaluate the kinetic parameters using the viscosity data at different cure temperatures under isothermal conditions As the storage modulus, G' is proportional to the chemical cross links and becomes significant only after the g<4 point, it was used to follow the changes in conversion known as rheoconversion after the gel point The rheoconversion was found by normalizing the G' data with G1^, the storage modulus of the fully cured resin It was used to study the cuie kinetics using an autocatalytic model The kinetic parameters such as rate constant, acceptation and retardation parameters were evaluated and that temperature dependence was established. While the existing models relate viscosity and conversion only up to gel point the new proposed model, termed VISCON model takes into account the changes up to vitrification. The relation so developed is used to modify the autocatalytic cure model based on chemical conversion. The parameters appearing in this model were evaluated using Levenberg-Marquardt error minimization algorithm. The kinetic parameters obtained are comparable with the values estimated using the DSC data. All the models cited above represent the microkinetic aspects. The models based on the information of TTT cure diagrams, however, represent the macrokinetic aspects of the cure, as they are based on the cure stages such as gelation and vitrification TTT diagram relates the cure characteristics like cure temperature, cure time, Ta and, indirectly, chemical conversion Hence the ultimate properties of the composite could he predicted and established with the help of the models based on TTT cure diagrams The changes in the storage modulus, G1 and loss modulus, G", were followed to identify the gel and vitrification points of the resin systems at different cure temperatures Gel point and vitrification point were used to generate gelation and vitrification hues in the construction of TTT cure diagrams for EPN/DDM, TGPAP/TDA and TGDDM/PDA resin systems Theoretical TTT diagrams were generated and IBO-T, contours were established using the TTT diagram-based models The cure schedule for the resin systems investigated could be determined from the TTT diagram and the respective rheological data.
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43

Paez, Espejo Miguel angel. "Modélisation et simulation du comportement spatiotemporel des transitions de phase dans les monocristaux moléculaires à transition de spin." Thesis, Université Paris-Saclay (ComUE), 2016. http://www.theses.fr/2016SACLV034/document.

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Ce travail est dédié à la modélisation multi-échelle des phénomènes liés à la transition de spin dans des composés du Fe(II). Le développement d'un modèle macroscopique type réaction-diffusion pour la transition de phase à partir de l'Hamiltonien d'Ising a permis l'étude théorique des aspects spatio-temporels de la fraction haut-spin lors de la transition de phase du premier ordre dans des monocristaux commutables. La comparaison à l'expérience a conduit à de très bons accords pour le comportement du front de transition, ce qui a permis de mieux comprendre les mesures de microscopie optique. Ce travail a été étendu à l'étude des effets photo-thermiques qui causent l'échauffement du cristal par la lumière du microscope conduisant à un système d'équations différentielles couplées tenant compte du couplage thermique avec le bain.Ces équations prédisent des comportements non-linéaires du cristal dans son domaine bistable, tels que l’existence d’effets autocatalytiques, dont les conditions d'émergence ont été précisées. La dernière partie de la thèse est consacrée à une extension du modèle électro-élastique. Ici on démontre que la frustration élastique est à l'origine de la transition de spin en deux étapes et des transitions incomplètes. Ceci nous a amené aussi à prédire l'organisation de structures complexes de la fraction haut-spin dans les phases intermédiaires. Plusieurs types d'auto-organisation ont été révélés dont des structures modulées de la fraction haut-spin. Ce type de comportements a été observé expérimentalement très récemment dans les composés à transition de spin
This work is devoted to the multiscale modeling of the spin transition phenomena in Fe(II) spin crossover compounds. The development of a macroscopic reaction-diffusion-like model for the phase transition from the Ising-like Hamiltonian allowed the theoretical study of the spatio-temporal behavior of the high-spin fraction accompanying the first-order phase transition in switchable spin crossover single crystals. The comparison to experiments led to an excellent agreement for the dynamics of the high-spin/low-spin interface which improved the understanding of the optical microscopy measurements. Next, this work was extended to the study of photothermic effects due to the crystal heating by the light of the microscope leading to a coupled system of differential equations accounting for the thermal coupling with the bath temperature. These equations predict nonlinear behaviors for crystals in the bistable region, such as the autocatalytic effects, for which we established the conditions of their emergence. The last part of this thesis is devoted to an extension of the electro-elastic model. Here we prove that the elastic frustration is at the origin of the existence of two-step and of incomplete spin crossover transitions. Furthermore, this model allowed us to predict structures of complex patterns in high-spin fractions for intermediate phases. Several types of self-organisation were revealed such as the spatially-modulated structures of the high-spin fractions. Some of these behaviors have been experimentally observed, very recently, in spin crossover compounds
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44

Eickes, Christian. "Die autokatalytische H 2 O 2 -Reduktion an Ag-Elektroden." Doctoral thesis, Humboldt-Universität zu Berlin, Mathematisch-Naturwissenschaftliche Fakultät I, 2001. http://dx.doi.org/10.18452/14597.

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Es konnte vor kurzem gezeigt werden, daß die Reduktion von Wasserstoffperoxid (H2O2) an Silber in Perchlorsäure (HClO4) über zwei parallele Wege verläuft. Die normale Reduktion wird bei einer Überspannung von -1,5 V beobachtet, während die zweite Reduktionsreaktion bei einer deutlich geringeren Überspannung bei -1,0 V stattfindet. Im zweiten Reaktionsweg wird OHad als instabile Zwischenspezies gebildet und wirkt katalytisch auf die H2O2-Reduktion. Daher wird angenommen, daß die zweite Reaktion eine autokatalytische Reduktion ist. Diese autokatalytische Reaktion wird nach einer ge-wissen Zeit deaktiviert, die von der Rotationsgeschwindigkeit der Elektrode abhängig ist. Sie kann wiedererlangt werden, wenn die Elektrode negativ polarisiert wird. In dieser Arbeit wurden Ex-situ-XPS-Messungen an herausgezogenen Ag(111)-Elektroden durch-geführt. Die Analyse führt zu dem Ergebnis, daß die Deaktivierung durch geringe Chlorid-Verunreinigungen verursacht wird. Elektrochemische Impedanzspektren werden zusammen mit numerischen Simulationen der Faradayschen Impedanz des autokata-lytischen Bereiches gezeigt. Diese basieren auf Annahmen von kinetischen Geschwin-digkeitsgesetzen, die früher postuliert wurden. Die experimentellen Daten stimmen sehr gut mit den Ergebnissen der theoretischen Rechnungen überein. Dies unterstützt den angenommen autokatalytischen Mechanismus.
Recently, it was shown that the hydrogen peroxide (H2O2) reduction on silver in perchloric acid (HClO4) proceeds in two parallel paths. The normal reduction is observed at an overpotential of -1.5 V, whereas a second reduction reaction occurs at a significantly lower overpotential at -1.0 V. The second reaction involves the unstable intermediate OHad, which also acts as a catalyst. Hence, the second reaction has been proposed to be an autocatalytic one. This autocatalytic reaction is deactivated after a certain time that depends on the rotation speed of the electrode. It can be recovered if the electrode is negatively polarized. In this thesis work, ex-situ XPS measurements on emersed Ag(111) electrodes were conducted. The analysis leads to the conclusion that the deactivation is caused by a small amount of chloride contamination. Electrochemical impedance spectra are presented together with numerical simulations for the faradaic impedance in the autocatalytic region based on previously suggested kinetic rate laws. The experimental data fit well with the results of the theoretical calculations, which strongly supports the autocatalytic mechanism.
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45

Eilerts, Diane. "Recombinant Expression and Potential Autocatalysis of Aedes aegypti Trypsin-Like Serine Proteases (AaSPII and AaSPIV)." Thesis, San Jose State University, 2017. http://pqdtopen.proquest.com/#viewpdf?dispub=10284010.

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Aedes aegypti mosquitoes can be found globally in tropical and subtropical urban areas and spread Zika, Dengue fever, yellow fever, and Chikungunya viruses. Current vector control methods are limited and nonspecific. The female Ae. aegypti mosquito uses blood meal proteins to obtain nutrients required for oogenesis; inhibition of the midgut trypsin-like serine proteases responsible for blood meal digestion may provide a novel method of vector control. Ae. aegypti blood meal digestion is complex and the role of uncharacterized serine proteases in blood digestion is unclear; specifically, a group of trypsin-like serine proteases (AaSPII–V) is expressed at constant levels before and following Ae. aegypti blood meal acquisition. This research focuses on the in vitro biochemical study of two specific Ae. aegypti trypsin-like serine proteases (AaSPII and AaSPIV) in order to gain further understanding of their role in blood meal digestion. The approach involved the successful cloning and bacterial expression of these soluble, recombinant proteases. Results from attempts to purify these proteases were unsuccessful but indicative of potential autocatalytic and autodigestive behavior. Future studies will focus on obtaining purified recombinant proteases for further study. The study of AaSPII and AaSPIV, as well as other midgut Ae. aegypti proteases, will aid in understanding the overall role proteases play in blood meal digestion and may eventually allow for the development of mosquito-specific enzyme inhibitors.

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46

Poletti, Patrick David. "The Effect of Dynamic Kinetic Selection on an Evolving Ribozyme Population." Thesis, Portland State University, 2019. http://pqdtopen.proquest.com/#viewpdf?dispub=13422098.

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Dynamic Kinetic Selection (DKS) suggests that kinetic, rather than thermodynamic, stability will dictate the composition of a replicating population of biomolecules. Here, the results obtained from a series of five related reactions involving gradually increasing percentages of randomly-mutated substrate fragments to generate variants of full-length Azoarcus group I intron through an autocatalytic self-assembly reaction involving a series of recombination events, showed DKS as a driving factor in dictating the population composition of full-length product assembled from substrates that had fewer positions available to randomization.

In trying to elucidate a plausible scheme for the origins of complex biomolecules on the prebiotic Earth, the suggestion that networks comprised of interacting molecules were more likely to evolve into biomolecules capable of obtaining and sustaining characteristics attributed to living molecules has gained traction within the past few years. Of specific interest is the catalytic efficacy of ribozymes whose genotypes require that they interact with molecules of the same genotype (selfish systems) to be effective catalysts versus those that are more effective when accomplishing catalysis by cooperating with ribozymes of a different genotype (cooperative systems). Here, the Azoarcus I ribozyme was used to compare these two types of system. Both systems were shown to robustly produce full-length product. Two different methods of introducing random mutations into substrate fragments for the reactions described in this thesis were employed. The differences in the preparation methods for the substrates was not expected to have an impact on the nature of the full-length product. However, there was no correlation between the positions that tended to be more tolerant of accepting random mutations between the products arising from the two preparation methods. One preparation method yielded full-length ribozymes more consistent with the secondary structure of the wild-type ribozyme and followed substitution patterns found in in vivo nucleic acid substitutions, whereas the other method provided full-length ribozymes that tolerated mutations that would be expected to greatly affect the secondary structure of the ribozyme and those positions tended to mutate evenly to any of the three possible alternative nucleobases.

Point mutations introduced into ribozyme substrate fragments may have a deleterious, neutral, or beneficial effect, depending on their impact on the catalytic capability of the molecule vis-á-vis the effect, if any, the change has to the secondary and tertiary structure of the ribozyme. In this dissertation, the results of two series of point mutation reactions are addressed. The first set showed a point mutation to have a deleterious effect, whereas concerted mutations did not significantly affect activity of the ribozyme. The second series of reactions involved point mutations at a position that had previously been determined to be highly tolerant of random mutations. Results suggested that substitutions at this position had a minimal impact on ribozyme activity.

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47

Rayder, Thomas M. "Modulation of Catalyst@MOF Host-Guest Composites in Pursuit of Synthetic Artificial Enzymes:." Thesis, Boston College, 2020. http://hdl.handle.net/2345/bc-ir:108930.

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Thesis advisor: Jeffery A. Byers
Thesis advisor: Chia-Kuang (Frank) Tsung
Biological systems have evolved over time to favor structures beneficial for the efficient transformation of simple feedstocks to sophisticated products. In particular, enzymes have evolved such that cooperative and geometrically controlled interactions between active sites and substrates enhance catalytic activity and selectivity. Separation of these active sites from other incompatible catalytic components allows for chemical transformation in a stepwise fashion, circumventing the inherent limitations to performing reactions in a single step. This dissertation describes the use of porous crystalline materials called metal-organic frameworks (MOFs) as hosts to mimic the component separation and precise active site control observed in nature. The first phase of these efforts explores the use of dissociative “aperture-opening” linker exchange pathways in a MOF to encapsulate transition metal complexes for carbon dioxide hydrogenation to formate. This strategy is then used to separate two incompatible complexes and perform the cascade conversion of carbon dioxide to methanol, resulting in unique and previously unobserved network autocatalytic behavior. Finally, the modularity of the MOF host is leveraged to install beneficial functionality in close proximity to the encapsulated transition metal complex, leading to activity exceeding that of any reported homogeneous system for carbon dioxide reduction. The insights gained through these studies can inform the development of composites for other reactions, allowing for access to new and unique reaction manifolds
Thesis (PhD) — Boston College, 2020
Submitted to: Boston College. Graduate School of Arts and Sciences
Discipline: Chemistry
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48

Uwaha, Makio, and Hiroyasu Katsuno. "Mechanism of Chirality Conversion by Grinding Crystals -Ostwald Ripening vs Crystallization of Chiral Clusters-." The Physical Society of Japan, 2009. http://hdl.handle.net/2237/13866.

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49

He, Lichun [Verfasser], and Christiane [Akademischer Betreuer] Ritter. "Structural basis for signaling in innate immunity via autocatalytical changes of MAVS by NMR / Lichun He ; Betreuer: Christiane Ritter." Braunschweig : Technische Universität Braunschweig, 2014. http://d-nb.info/1175820369/34.

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50

Uwaha, Makio. "Simple Models for Chirality Conversion of Crystals and Molecules by Grinding." The Physical Society of Japan, 2008. http://hdl.handle.net/2237/13865.

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