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HYDRATION AND phase separation OF TEMPERATURE-SENSITIVE WATER-SOLUBLE POLYMERS

Chinese Journal of Polymer Science 2011年第1期29卷 13-21页

作者： Fumihiko Tanaka Tsuyoshi Koga Hiroyuki Kojima Francoise M.Winnik Department of Polymer Chemistry Graduate School of EngineeringKyoto University Department of Chemistry and Faculty of Pharmacy University of Montréal

Collapse of a poly（N-isopropylacrylamide）（PNIPAM） chain upon heating and phase diagrams of aqueous PNIPAM solutions with very fiat lcst phase separation line are theoretically studied on the basis of cooperative dehydration （simultaneous dissociation of bound water molecules in a group of correlated sequence）, and compared with the experimental observation of temperature-induced coil-globule transition by light scattering methods. The transition becomes sharper with the cooperativity parameter σ of hydration. Reentrant coil-globule-coil transition in mixed solvent of water and methanol is also studied from the viewpoint of competitive hydrogen bonds between polymer-water and polymer-methanol. The downward shift of the cloud-point curves （lcst cononsolvency） with the mole fraction of methanol due to the competition is calculated and compared with the experimental data. Aqueous solutions of hydophobically-modified PNIPAM carrying short alkyl chains at both chain ends （telechelic PNIPAM） are theoretically and experimentally studied. The lcst of these solutions is found to shift downward along the sol-gel transition curve as a result of end-chain association （association-induced phase separation）, and separate from the coil-globule transition line. Associated structures in the solution, such as flower micelles, mesoglobules and higher fractal assembly, are studied by USANS with theoretical modeling of the scattering function.

关键词： Cooperative dehydration lcst phase separation Poly(N-isopropylacrylamide) Cononsolvency Coil-globule transition Flower micelle.

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