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Hierarchical Biomolecular Emulsions Using 3-D Microfluidics with Uniform Surface Chemistry
Biomacromolecules ( IF 5.5 ) Pub Date : 2017-10-19 00:00:00 , DOI: 10.1021/acs.biomac.7b01159
Zenon Toprakcioglu 1 , Aviad Levin 1 , Tuomas P. J. Knowles 1, 2
Affiliation  

Microfluidic devices can be used to produce single, double and higher order emulsions, where droplet sizes can be precisely controlled and modulated. Such emulsions have great potential for the storage and study of biomolecules, including peptides and proteins. However, advancement of this technique has remained challenging due to the tendency of various biomolecules to adhere to the surface of the formed channels, resulting in changes in surface wetting and fouling on the micrometer scale. Thus, precise control of surface wettability plays a crucial role in the processes that govern droplet formation. Here, we report an approach for producing both water–oil–water (w/o/w) and oil–water–oil (o/w/o) double emulsions without any need for surface modification, an enabling feature for biomolecular encapsulation. Using this strategy, we show that the number of monodisperse encapsulated internal droplets can be controlled systematically and reproducibly by suitable adjustment of the relevant flow rates, and ranges from 1 to 40 in the case of w/o/w emulsions. We further demonstrate that the number of internal droplets scales linearly with the reciprocal flow rate of the outer continuous phase, when the inner and middle phase flow rates are kept constant. We demonstrate that this approach is suitable for forming double emulsions where the inner phase consists of reconstituted silk protein solution whereby incubation of the internal droplets can be induced to form a gel resulting in silk fibroin microgels surrounded by an external oil shell. Finally, for o/w/o emulsions, we show that single or multiple monodisperse internal droplets can be encapsulated with a size that ranges over 1 order of magnitude, from ca. 10 μm to >100 μm. Moreover, o/w/o emulsions where the middle phase consists of silk fibroin solution were prepared and by allowing the protein to aggregate, a core–shell structure was formed. This microfluidic strategy allows for multiple emulsions to be generated drop by drop for biomolecular solutions with potential applications in the biomedical and pharmaceutical fields.

中文翻译:

使用3-D微流控技术和均匀表面化学的分层生物分子乳液

微流控设备可用于生产单,双和更高阶的乳液,可精确控制和调节液滴大小。这样的乳剂对于存储和研究包括肽和蛋白质的生物分子具有巨大的潜力。然而,由于各种生物分子倾向于粘附在形成的通道的表面上,导致微米级的表面润湿和结垢变化,因此该技术的进步仍然具有挑战性。因此,表面润湿性的精确控制在控制液滴形成的过程中起着至关重要的作用。在这里,我们报告了一种无需进行表面改性即可生产水-油-水(w / o / w)和油-水-油(o / w / o)双重乳液的方法,这是生物分子封装的一个有利功能。使用这种策略,我们表明,通过适当调节相关的流速,可以系统地和可重复地控制单分散包封的内部液滴的数量,在w / o / w乳液的情况下,其范围为1至40。我们进一步证明,当内部和中间相流速保持恒定时,内部液滴的数量与外部连续相的往复流速成线性比例。我们证明该方法适用于形成内相由重构的丝蛋白溶液组成的双乳剂,从而可以诱导内部液滴的孵育以形成凝胶,从而形成被外部油壳包围的丝素蛋白微凝胶。最后,对于o / w / o乳液,我们表明,单个或多个单分散内部液滴可以以大约1个数量级的大小封装。10μm至> 100μm。此外,制备了中间相由丝素蛋白溶液组成的o / w / o乳液,通过使蛋白质聚集,形成了核-壳结构。这种微流体策略允许逐滴产生多种乳液,用于生物分子溶液,在生物医学和制药领域具有潜在的应用。
更新日期:2017-10-20
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