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Structural reorganization of cylindrical nanoparticles triggered by polylactide stereocomplexationSun, L., Pitto-Barry, Anaïs, Kirby, N., Schiller, T.L., Sanchez, A.M., Dyson, M.A., Sloan, J., Wilson, N.R., O'Reilly, R.K., Dove, A.P. 17 December 2014 (has links)
Yes / Co-crystallization of polymers with different configurations/tacticities provides access to materials with enhanced performance. The stereocomplexation of isotactic poly(L-lactide) and poly(D-lactide) has led to improved properties compared with each homochiral material. Herein, we report the preparation of stereocomplex micelles from a mixture of poly(L-lactide)-b-poly(acrylic acid) and poly(D-lactide)-b-poly(acrylic acid) diblock copolymers in water via crystallization-driven self-assembly. During the formation of these stereocomplex micelles, an unexpected morphological transition results in the formation of dense crystalline spherical micelles rather than cylinders. Furthermore, mixture of cylinders with opposite homochirality in either THF/H2O mixtures or in pure water at 65 °C leads to disassembly into stereocomplexed spherical micelles. Similarly, a transition is also observed in a related PEO-b-PLLA/PEO-b-PDLA system, demonstrating wider applicability. This new mechanism for morphological reorganization, through competitive crystallization and stereocomplexation and without the requirement for an external stimulus, allows for new opportunities in controlled release and delivery applications. / University of Warwick, Swiss National Science Foundation and the EPSRC. The Royal Society - an Industry Fellowship to A.P.D. The Engineering and Physical Sciences Research Council (EP/G004897/1) - funding to support postdoctoral fellowships for A.P.B. as well as funding for J.S. and M.A.D. through the Warwick Centre for Analytical Science (EP/F034210/1). The Science City Research Alliance and the HEFCE Strategic Development Fund - funding support. Some items of equipment that were used in this research were funded by Birmingham Science City, with support from Advantage West Midlands and part-funded by the European Regional Development Fund.
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SHEAR RHEOMETRY PROTOCOLS TO ADVANCE THE DEVELOPMENT OF MICROSTRUCTURED FLUIDSEduard Andres Caicedo Casso (6620462) 15 May 2019 (has links)
<p></p><p>This doctoral dissertation takes the reader through a
journey where applied shear rheology and flow-velocimetry are used to
understand the mesoscopic factors that control the flow behavior of three
microstructured fluids. Three individual protocols that measure relative
physical and mechanical properties of the flow are developed. Each protocol
aims to advance the particular transformation of novel soft materials into a
commercial product converging in the demonstration of the real the chemical,
physical and thermodynamical factors that could potentially drive their
successful transformation. </p>
<p> </p>
<p>First, this dissertation introduces the use of rotational
and oscillatory shear rheometry to quantify the solvent evaporation effect on
the flow behavior of polymer solutions used to fabricate isoporous asymmetric
membranes. Three different A-B-C triblock copolymer were evaluated:
polyisoprene-<i>b</i>-polystyrene-<i>b</i>-poly(4-vinylpyridine) (ISV);
polyisoprene-<i>b</i>-polystyrene-<i>b</i>-poly(<i>N</i>,<i>N</i>-dimethylacrylamide)
(ISD); and polyisoprene-<i>b</i>-polystyrene-<i>b</i>-poly(<i>tert</i>-butyl methacrylate) (ISB). The resulting evaporation-induced
microstructure showed a solution viscosity and film viscoelasticity strongly
dependent on the chemical structure of the triblock copolymer molecules. </p>
<p> </p>
<p>Furthermore, basic shear rheometry, flow birefringence, and
advanced flow-velocimetry are used to deconvolute the flow-microstructure relationships
of concentrated surfactant solutions. Sodium laureth sulfate in water (SLE<sub>1</sub>S)
was used to replicate spherical, worm-like, and hexagonally packed micelles and
lamellar structures. Interesting findings demonstrated that regular features of
flow curves, such as power-law shear thinning behavior, resulted from a wide
variety of experimental artifacts that appeared when measuring microstructured
fluids with shear rheometry.</p>
<p> </p>
<p>Finally, the successful integration of shear rheometry to
calculate essential parameters to be used in a cost-effective visualization
technique (still in development) used to calculate the dissolution time of
polymers is addressed. The use of oscillatory rheometry successfully quantify
the viscoelastic response of polyvinyl alcohol (PVA) solutions and identify
formulations changes such as additive addition. The flow behavior of PVA
solutions was correlated to dissolution behavior proving that the developed
protocol has a high potential as a first screening tool.</p><br><p></p>
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