College of Chemistry, Research Center for Analytical Sciences, and Tianjin Key Laboratory of Molecular Recognition and Biosensing , Nankai University , Tianjin 300071 , China.
State Key Laboratory of Medicinal Chemical Biology , Nankai University , Tianjin 300071 , China.
ACS Nano. 2019 Feb 26;13(2):1421-1432. doi: 10.1021/acsnano.8b07054. Epub 2019 Feb 11.
Self-assembly is a powerful tool to organize the elementary molecular units into functional nanostructures, which provide reversible stimulus-responsive systems for a variety of purposes. However, the ability to modulate the reversible self-assembly in live systems remains a great challenge owing to the chemical complexity of intracellular environments, which often damage synthetic assembled superstructures. Herein, we describe a robust reversible self-assembly system that is composed of a hydrophobic gold nanoparticle (AuNP) core and a shell of pH-responsive dye-incorporated block copolymers. The reversible assembly-disassembly processes were precisely controlled through mediating the molecular interactions between the copolymers and AuNPs. More importantly, the major endogenous biospecies such as proteins will not impair the reversible self-assembly, which was supported by free-energy calculations. The reversible pH-responsive nanostructures were employed as "smart" probes for visualizing the subtle dynamic pH changes among different intracellular compartments, facilitating the study of pH influence on biological processes.
自组装是一种将基本分子单元组织成功能纳米结构的强大工具，为各种目的提供了具有可逆刺激响应的系统。然而，由于细胞内环境的化学复杂性，调节活系统中可逆自组装的能力仍然是一个巨大的挑战，因为细胞内环境常常会破坏合成组装的超结构。在此，我们描述了一种由疏水性金纳米粒子（AuNP）核心和 pH 响应染料掺入的嵌段共聚物外壳组成的稳健的可逆自组装系统。通过调节共聚物和 AuNPs 之间的分子相互作用，精确地控制了可逆的组装-解组装过程。更重要的是，主要的内源性生物物质，如蛋白质，不会损害可逆自组装，这得到了自由能计算的支持。可逆 pH 响应纳米结构可用作可视化不同细胞内隔室之间微妙动态 pH 变化的“智能”探针，有助于研究 pH 对生物过程的影响。
