Preparative Macromolecular Chemistry, Institut für Technische Chemie und Polymerchemie, Karlsruhe Institute of Technology (KIT) , Engesserstraße 18, 76128 Karlsruhe, Germany.
Institut für Biologische Grenzflächen, Karlsruhe Institute of Technology (KIT) , Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany.
J Am Chem Soc. 2017 Jan 11;139(1):51-54. doi: 10.1021/jacs.6b10952. Epub 2016 Dec 27.
Herein, we introduce the first approach to map single-chain nanoparticle (SCNP) folding via high-resolution electrospray ionization mass spectrometry (ESI MS) coupled with size exclusion chromatography. For the first time, the successful collapse of polymeric chains into SCNPs is imaged by characteristic mass changes, providing detailed mechanistic information regarding the folding mechanism. As SCNP system we employed methyl methacrylate (MMA) statistically copolymerized with glycidyl methacrylate (GMA), resulting in p(MMA-stat-GMA), subsequently collapsed by using B(CF) as catalyst. Both the precursor polymer and the SCNPs can be well ionized via ESI MS, and the strong covalent cross-links are stable during ionization. Our high-resolution mass spectrometric approach can unambiguously differentiate between two mechanistic modes of chain collapse for every chain constituting the SCNP sample.
在这里，我们介绍了一种通过高分辨率电喷雾电离质谱（ESI-MS）与尺寸排阻色谱相结合来绘制单链纳米颗粒（SCNP）折叠的方法。通过特征质量变化，首次成功地将聚合物链折叠成 SCNP，为折叠机制的详细机制信息提供了依据。我们采用甲基丙烯酸甲酯（MMA）与甲基丙烯酸缩水甘油酯（GMA）的统计共聚物作为 SCNP 体系，得到 p（MMA-stat-GMA），然后用 B（CF）作为催化剂使其折叠。ESI-MS 可以很好地对前体聚合物和 SCNP 进行离子化，并且在离子化过程中强共价交联是稳定的。我们的高分辨率质谱方法可以明确地区分构成 SCNP 样品的每条链的两种链折叠的机制模式。
