Lin Chenyu, Katla Sai Krishna, Pérez-Mercader Juan
Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, United States.
The Santa Fe Institute, Santa Fe, NM, United States.
Commun Chem. 2021 Feb 26;4(1):25. doi: 10.1038/s42004-021-00464-8.
Autonomous and out-of-equilibrium vesicles synthesised from small molecules in a homogeneous aqueous medium are an emerging class of dynamically self-assembled systems with considerable potential for engineering natural life mimics. Here we report on the physico-chemical mechanism behind a dynamic morphological evolution process through which self-assembled polymeric structures autonomously booted from a homogeneous mixture, evolve from micelles to giant vesicles accompanied by periodic growth and implosion cycles when exposed to oxygen under light irradiation. The system however formed nano-objects or gelation under poor oxygen conditions or when heated. We determined the cause to be photoinduced chemical degradation within hydrated polymer cores inducing osmotic water influx and the subsequent morphological dynamics. The process also led to an increase in the population of polymeric objects through system self-replication. This study offers a new path toward the design of chemically self-assembled systems and their potential application in autonomous material artificial simulation of living systems.
在均匀水介质中由小分子合成的自主且非平衡囊泡是一类新兴的动态自组装系统，在构建天然生命模拟物方面具有巨大潜力。在此，我们报告了一个动态形态演化过程背后的物理化学机制，通过该过程，从均匀混合物中自主启动的自组装聚合物结构，在光照下暴露于氧气时，会从胶束演变为巨型囊泡，并伴随着周期性的生长和内爆循环。然而，该系统在低氧条件下或加热时会形成纳米物体或发生凝胶化。我们确定其原因是水合聚合物核内的光诱导化学降解，导致渗透水流入以及随后的形态动力学变化。该过程还通过系统自我复制导致聚合物物体数量增加。这项研究为化学自组装系统的设计及其在生命系统自主材料人工模拟中的潜在应用提供了一条新途径。
