Maag Patrick H, Feist Florian, Frisch Hendrik, Roesky Peter W, Barner-Kowollik Christopher
School of Chemistry and Physics, Queensland University of Technology (QUT) 2 George Street QLD 4000 Brisbane Australia.
Centre for Materials Science, Queensland University of Technology (QUT) 2 George Street QLD 4000 Brisbane Australia
Chem Sci. 2024 Feb 28;15(14):5218-5224. doi: 10.1039/d3sc06651g. eCollection 2024 Apr 3.
Single chain nanoparticles (SCNPs) are a highly versatile polymer architecture consisting of single polymer chains that are intramolecularly crosslinked. Currently, SCNPs are discussed as powerful macromolecular architectures for catalysis, delivery and sensors. Herein, we introduce a methodology based on Förster Resonance Energy Transfer (FRET) to evidence the folding of single polymer chains into SCNPs fluorescence readout. We initially introduce a molecular FRET pair based on a bimane and nitrobenzoxadiazole (NBD) moiety and study its fluorescence properties in different solvents. We subsequently construct a low dispersity polymer chain carrying NBD units, while exploiting the bimane units for intramolecular chain collapse. Upon chain collapse and SCNP formation - thus bringing bimane and NBD units into close proximity - the SCNPs report their folded state by a strong and unambiguous FRET fluorescence signal. The herein introduced reporting of the folding state of SCNPs solely relies on an optical readout, opening avenues to monitoring SCNP folding without recourse to complex analytical methodologies.
单链纳米颗粒（SCNPs）是一种高度通用的聚合物结构，由分子内交联的单聚合物链组成。目前，SCNPs被认为是用于催化、递送和传感的强大高分子结构。在此，我们介绍一种基于Förster共振能量转移（FRET）的方法，以通过荧光读数证明单聚合物链折叠成SCNPs。我们首先引入基于双硫烷和硝基苯并恶二唑（NBD）部分的分子FRET对，并研究其在不同溶剂中的荧光性质。随后，我们构建了一条携带NBD单元的低分散聚合物链，同时利用双硫烷单元实现分子内链塌陷。在链塌陷和SCNP形成时——从而使双硫烷和NBD单元紧密靠近——SCNPs通过强烈且明确的FRET荧光信号报告其折叠状态。本文介绍的SCNPs折叠状态报告仅依赖于光学读数，为监测SCNP折叠开辟了途径，而无需借助复杂的分析方法。
