Multiple Levels of Organization in Amphiphilic Diblock Copolymers Based on Poly(γ-benzyl‑l‑glutamate) Produced by Aqueous ROPISA

IF 5.4 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Biomacromolecules Pub Date : 2025-03-10 DOI:10.1021/acs.biomac.4c01657

Marianna Spyridakou , Ioannis Tzourtzouklis , Robert Graf , Hannah Beauseroy , Colin Bonduelle , Sebastien Lecommandoux , George Floudas

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Abstract

A recent method for producing amphiphilic block copolymers and nano-objects based on the ring-opening polymerization-induced self-assembly (ROPISA) in aqueous buffer is explored with respect to the tunability toward nanostructures. ROPISA gives rise to polypeptide copolymers with unprecedented levels of organization. By employing amphiphilic block copolymers of poly(ethylene glycol) (PEG) with the synthetic polypeptide poly(γ-benzyl-l-glutamate) (PBLG) and a combination of static (¹³C NMR, X-ray scattering, polarizing optical microscopy), thermodynamic (differential scanning calorimetry), and dynamic (dielectric spectroscopy) probes, we demonstrate a record of six levels of organization only found before in natural materials. These levels of organization could not be obtained in earlier morphology investigations of copolymers based on PEG and PBLG prepared by different methods. Furthermore, the type of NCA monomer (BLG-NCA vs Leu-NCA) and the solvent treatment method had an influence on the degree of segregation, the α-helical content, and the order-to-disorder transition temperature in the PEG-b-PBLG and PEG-b-PLeu copolymers.

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基于聚（γ-苄基-谷氨酸）的两亲性双嵌段共聚物的多级组织

研究了一种基于开环聚合诱导自组装（ROPISA）的两亲嵌段共聚物和纳米共聚物的制备方法，并探讨了其对纳米结构的可调性。ROPISA产生的多肽共聚物具有前所未有的组织水平。通过使用聚乙二醇（PEG）的两亲嵌段共聚物与合成多肽聚γ-苄基-谷氨酸（PBLG）以及静态（13C NMR， x射线散射，偏光显微镜），热力学（差示扫描量热法）和动态（介电光谱）探针的组合，我们展示了六个级别的组织记录，这些记录以前只在天然材料中发现过。这些水平的组织不能在早期的形貌研究中获得基于PEG和PBLG的共聚物通过不同的方法制备。此外，NCA单体类型（BLG-NCA vs Leu-NCA）和溶剂处理方式对PEG-b-PBLG和PEG-b-PLeu共聚物的偏析程度、α-螺旋含量和有序-无序转变温度都有影响。

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来源期刊

Biomacromolecules 化学-高分子科学

CiteScore

10.60

自引率

4.80%

发文量

417

审稿时长

1.6 months

期刊介绍： Biomacromolecules is a leading forum for the dissemination of cutting-edge research at the interface of polymer science and biology. Submissions to Biomacromolecules should contain strong elements of innovation in terms of macromolecular design, synthesis and characterization, or in the application of polymer materials to biology and medicine. Topics covered by Biomacromolecules include, but are not exclusively limited to: sustainable polymers, polymers based on natural and renewable resources, degradable polymers, polymer conjugates, polymeric drugs, polymers in biocatalysis, biomacromolecular assembly, biomimetic polymers, polymer-biomineral hybrids, biomimetic-polymer processing, polymer recycling, bioactive polymer surfaces, original polymer design for biomedical applications such as immunotherapy, drug delivery, gene delivery, antimicrobial applications, diagnostic imaging and biosensing, polymers in tissue engineering and regenerative medicine, polymeric scaffolds and hydrogels for cell culture and delivery.