Facile, one-step synthesis of self-assembling, cationic block copolymers of poly(2-N-(dimethylaminoethyl) methacrylate) (pDMAEMA) and PEO-PPO-PEO (Pluronic®) is developed. The copolymers are obtained via free-radical polymerization of DMAEMA initiated by Pluronic-radicals generated by cerium (IV). The copolymers possess surface activity, are polycationic at pH<7.1, and self-assemble into micelle-like aggregates when neutralized. Potential applications of the novel copolymers for DNA transfection in gene therapy are discussed. / Singapore-MIT Alliance (SMA)

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A new reactor and a novel in-situ sampling technique were developed for the study of the synthesis of Ce02 powders produced from dissolved cerium nitrate salts. The reactor minimized particle recirculation and provided a highly symmetric and undisturbed plasma flow suitable for the analysis of the phenomena affecting the formation of Ce02 powders. The sampling probe provided in-situ sampling of in-flight CeCb particles and allowed continuous sampling without cross contamination. The sampled particles were collected using a wet collection system composed of a mist atomizer acting as a scrubber and a custom-made spray chamber. The entire collection system is portable and it was tested in the particle range of 20 nm to 100 jam. This information provided a picture of how Ce02 particles were formed. A numerical simulation of different plasma operating parameters using Fluent was presented. A comprehensive droplet-to-particle formation mechanism was deduced based on calorimetry. thermodynamics of Ce02 formation, numerical simulations and collected particles. The effect of adding water soluble fuels (alanine and glycine) to the original cerium nitrate solutions was investigated. Fuel addition decreased the temperature of CeC>2 formation by acting as a local heat source as a result of fuel auto-ignition. The addition of fuel caused “particle size discrimination’*, and a single mode particle size distribution centered between 50-140 nm was achieved along the centerline of the reactor. [...] / Un nouveau reacteur et une technique innovatrice d’echantillonnage in situ furent developpes pour etudier la synthese de poudres de Ce02 produites a partir de sels de nitrate de cerium dissous. Le reacteur minimise la recirculation des particules et fournit un plasma non perturbe et grandement symetrique approprie pour l’analyse des phenomenes affectant la formation de poudres de Ce02. De plus, une sonde permet un echantillonnage in situ et en vol des particules de Ce02 et ce, en continu et sans contamination croisee. Les particules ainsi captees sont recueillies grace a un systeme de collecte par voie humide qui est compose d’un atomiseur de brume (mist atomizer) qui joue le role d’un recureur (scrubber) et d’une chambre d’atomisation (spray chamber) maison. Le systeme d’echantillonnage est mobile et fut teste sur des particules ayant des tailles de 20 nm a 100 jam. C’est grace a l’analyse des particules ainsi recueillies que nous sommes en mesure de comprendre comment les particules de Ce02 sont formees. Nous presentons aussi une simulation numerique, effectuee avec le logiciel Fluent, qui utilise les differents parametres d’experimentation. Le mecanisme detaille de la formation des particules a partir de gouttelettes fut deduit grace a des etudes calorimetriques, a une etude thermodynamique de la formation du Ce02, a des simulations numeriques et a l’analyse des particules recueillies. Nous avons aussi etudie l’effet d’un ajout de combustibles hydrosolubles (l’alanine et la glycine) a la solution originale de nitrate de cerium. Cette addition de combustibles diminue la temperature de formation du Ce02 en agissant comme une source locale de chaleur resultant de 1’auto-ignition du combustible. Aussi, le combustible cause une « segregation des particules » selon leur taille.

A new reactor and a novel in-situ sampling technique were developed for the study of the synthesis of CeO2 powders produced from dissolved cerium nitrate salts. The reactor minimized particle recirculation and provided a highly symmetric and undisturbed plasma flow suitable for the analysis of the phenomena affecting the formation of CeO2 powders. The sampling probe provided in-situ sampling of in-flight CeO2 particles and allowed continuous sampling without cross contamination. The sampled particles were collected using a wet collection system composed of a mist atomizer acting as a scrubber and a custom-made spray chamber. The entire collection system is portable and it was tested in the particle range of 20 nm to 100 mum. This information provided a picture of how CeO2 particles were formed. A numerical simulation of different plasma operating parameters using Fluent was presented. A comprehensive droplet-to-particle formation mechanism was deduced based on calorimetry, thermodynamics of CeO2 formation, numerical simulations and collected particles. The effect of adding water soluble fuels (alanine and glycine) to the original cerium nitrate solutions was investigated. Fuel addition decreased the temperature of CeO2 formation by acting as a local heat source as a result of fuel auto-ignition. The addition of fuel caused "particle size discrimination", and a single mode particle size distribution centered between 50-140 nm was achieved along the centerline of the reactor. / Also, heat and mass transfer effects were numerically investigated in evaporating solution droplets (20-40 mum in diameter) containing dissolved hexahydrated cerium nitrate in a stationary rf Ar-O2 thermal plasma. This model was developed to study the evaporation of a solution droplet surrounded by a porous crust in a stagnant rf Ar-O2 thermal plasma under reduced pressure. It considered a three phase system: a liquid core of dissolved Ce(NO 3)3.6H2O in water, a dry porous crust of homogeneously precipitated spherical crystals of equal size, and an Ar-O2 plasma under reduced pressure. The impact of different plasma operating parameters on the temperature and dissolved solid content profiles in the droplet was studied, i.e. surrounding plasma temperature, initial salt content and droplet size, plasma gas composition, and system pressure. Temperature and composition dependant thermophysical properties were used. The model was solved in a moving boundary frame using an ALE approach and considering Stefan flow. It provided the necessary information to understand the droplet to particle transformation steps in regions where in-flight probing was unfeasible, i.e. torch zone.

Thesis (Ph.D.)--Tufts University, 2004. / Submitted to the Dept. of Chemical and Biological Engineering. Includes bibliographical references.