Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo, 060-8628, Japan.
Faculty of Engineering, Hokkaido University, Sapporo, 060-8628, Japan.
Angew Chem Int Ed Engl. 2021 Aug 9;60(33):18122-18128. doi: 10.1002/anie.202103969. Epub 2021 Jul 8.
Developing an efficient and versatile process to transform a single linear polymer chain into a shape-defined nanoobject is a major challenge in the fields of chemistry and nanotechnology to replicate sophisticated biological functions of proteins and nucleic acids in a synthetic polymer system. In this study, we performed one-shot intrablock cross-linking of linear block copolymers (BCPs) to realize single-chain nanoparticles (SCNPs) with two chemically compartmentalized domains (Janus-shaped SCNPs). Detailed structural characterizations of the Janus-shaped SCNP composed of polystyrene-block-poly(glycolic acid) revealed its compactly folded conformation and compartmentalized block localization, similar to the self-folded tertiary structures of natural proteins. Versatility of the one-shot intrablock cross-linking was demonstrated using several different BCP precursors. In addition, the Janus-shaped SCNP produce miniscule microphase-separated structures.
将单个线性聚合物链转化为具有特定形状的纳米物体的高效、通用的方法是化学和纳米技术领域的主要挑战，其目的是在合成聚合物体系中复制蛋白质和核酸等复杂的生物功能。在本研究中，我们对线性嵌段共聚物（BCP）进行了单步嵌段交联，实现了具有两个化学分区（Janus 形状的 SCNP）的单链纳米颗粒（SCNP）。由聚苯乙烯-嵌段-聚（乙醇酸）组成的 Janus 形状的 SCNP 的详细结构表征表明，其具有紧密折叠的构象和分区的嵌段定位，类似于天然蛋白质的自折叠三级结构。使用几种不同的 BCP 前体证明了单步嵌段交联的多功能性。此外，Janus 形状的 SCNP 产生微小的微相分离结构。
