Butler Michael F, Heppenstall-Butler Mary
Unilever Research and Development, Colworth House, Sharnbrook, Bedfordshire, MK44 1LQ United Kingdom.
Biomacromolecules. 2003 Jul-Aug;4(4):928-36. doi: 10.1021/bm0340319.
Small-angle light scattering, turbidity, and confocal laser scanning microscopy were used to study microstructure formation and evolution in a gelatin/dextran mixture. There was a time-delay of up to tens of minutes between reaching the quench temperature and the onset of phase separation, because demixing only occurred once a certain amount of ordering of the gelatin molecules, measured by polarimetry, was attained. The accompanying phenomenon of gelation retarded the development of the microstructure to different extents, depending on the quench temperature. At low temperatures, the structure was rapidly trapped in a nonequilibrium state with diffuse interfaces, characteristic of the early and intermediate stages of phase separation. At higher temperatures, coarsening continued for a certain amount of time before the structure was trapped. The duration of the coarsening period increased with increasing temperature and the interface between the phases became sharp, characteristic of the late stages of phase separation. Because the ordering process continued after the target quench temperature was reached, the effective quench depth continued to increase after the initial phase separation. At high quench temperatures, the system was able to respond to the thermodynamic requirements of the increasing effective quench depth by undergoing secondary phase separation to form a droplet morphology within the preexisting bicontinuous one.
采用小角光散射、浊度法和共聚焦激光扫描显微镜研究了明胶/右旋糖酐混合物中微观结构的形成与演变。在达到淬火温度和相分离开始之间存在长达数十分钟的时间延迟,这是因为只有当通过旋光法测量的明胶分子达到一定程度的有序排列时才会发生相分离。伴随的凝胶化现象在不同程度上延缓了微观结构的发展,这取决于淬火温度。在低温下,结构迅速被困在具有扩散界面的非平衡状态,这是相分离早期和中期的特征。在较高温度下,在结构被困之前,粗化会持续一段时间。粗化期的持续时间随着温度的升高而增加,并且相之间的界面变得清晰,这是相分离后期的特征。由于在达到目标淬火温度后有序化过程仍在继续,初始相分离后有效淬火深度继续增加。在高淬火温度下,系统能够通过进行二次相分离来响应有效淬火深度增加的热力学要求,从而在先前存在的双连续结构中形成液滴形态。