Self-Adaptive Synthesis of Non-Covalent Crosslinkers while Folding Single-Chain Polymers

Dawei Qi, Xuncheng Shi, Caihong Lin, Ferdinand Holzhausen, Liljeström Ville, Xun Sun, Jinghui Luo, Leena Pitkänen, Ya Zhu, Jessica Rosenholm, Sirpa Jalkanen, Jianwei Li

Forskningsoutput: TidskriftsbidragArtikelVetenskapligPeer review

Sammanfattning

Abstract Peptide folding is a dynamic process driven by non-covalent cross-linking leading to functional nanostructures for essential biochemical activities. However, replicating this process in synthetic systems is challenging due to the difficulty in mimicking nature?s real-time regulation of non-covalent crosslinking for single-chain polymer folding. Here, we address this by employing anionic dithiol building blocks to create macrocyclic disulfides as non-covalent crosslinkers that adapted to the folding process. Initially, small macrocycles facilitated a low degree folding of a polycation. Then, this preorganized structure catalysed the production of larger macrocycles that enhanced the folding conversely. The self-adaptive synthesis was verified through the encapsulation of an anticancer drug, showing an updated production distribution of non-covalent crosslinkers and maximizing drug-loading efficiency against drug-resistant cancer in vitro. Our research advances the understanding of molecular systems by exploring species evolution via the structural dynamics of polymer folding. Additionally, adaptive synthesis enables controlled, sequential folding of synthetic polymers, with the potential to mimic protein functions.
OriginalspråkEngelska
Artikelnummere202408670
TidskriftAngewandte Chemie International Edition
Volym136
Nummer38
DOI
StatusPublicerad - 16 sep. 2024
MoE-publikationstypA1 Tidskriftsartikel-refererad

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