writer：Jiayu Yu, Jianing Zhang, Jing Jin, Wei Jiang
keywords：DNA均聚物, 路径依赖, 亚稳态, 微胶囊, 微碗
source：期刊
specific source：ACS Macro Letters, 2023, 12(6), 685-689
Issue time：2023年

摘要：提出了一种路径依赖策略，通过分次加入正丁醇和乳化（振荡）操作，在软乳液模板（水包正丁醇）中帮助单链DNA聚腺嘌呤（poly(dA)）规避亚稳态，实现从微胶囊到微碗的形貌调控。第一阶段，通过第四次溶剂添加和振荡形成小微胶囊；第二阶段，通过第五次溶剂添加和振荡启动小微胶囊膨胀，使其进入新路径以规避亚稳态，渗透再平衡和振荡是克服能量壁垒的两个必要条件；第三阶段，膨胀微胶囊在正丁醇蒸发后屈曲并演化为微碗，达到全局自由能最小稳定态。相反，传统一次性溶剂添加和振荡路径无法获得微碗。这种动力学路径依赖策略规避了亚稳态，并通过自组装将DNA寡核苷酸塑造成所需结构。

Abstract：A pathway-dependent strategy is proposed to assist single-stranded DNA polyadenine (poly(dA)) in evading metastable states and to achieve morphological regulation from microcapsules to microbowls by fractional n-butanol addition and emulsification (shaking) in a soft emulsion template (water-in-n-butanol). The first stage is the formation of small microcapsules by a fourth solvent addition and shaking. The second stage is the expansion of the small microcapsules initiated by the fifth solvent addition and shaking, drawing them to a new pathway to evade metastable states. Osmotic re-equilibrium and shaking are two indispensable conditions for overcoming the energy barriers. The third stage is the buckling of the expanded microcapsules and the evolution into microbowls after the evaporation of n-butanol to reach a global free energy minimum stable state. Conversely, the conventional one-time solvent addition and shaking pathway do not obtain microbowls. This kinetics pathway-dependent strategy evades metastability and shapes DNA oligonucleotides into desired structures via self-assembly.

论文链接：https://doi.org/10.1021/acsmacrolett.3c00250