具有超高生物大分子负载效率的聚合物囊泡的两个原理：酸诱导的吸附和亲和力增强的吸引力。,Macromolecules

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具有超高生物大分子负载效率的聚合物囊泡的两个原理：酸诱导的吸附和亲和力增强的吸引力。
Macromolecules ( IF 5.1 ) Pub Date : 2020-05-13 , DOI: 10.1021/acs.macromol.0c00252
Shuai Chen _{1,

2} , Jianglei Qin ₃ , Jianzhong Du _{1,

2}

Affiliation

在此，提出了两种新颖的原理，用于明智地设计具有多种生物大分子超高负载效率的聚合物囊泡：（1）蛋白质的酸诱导吸附（AIA）和（2）核酸的亲和力增强吸引（AEA）。前一种原理（AIA）由聚合物囊泡膜中的三唑基团辅助。后一种原理（AEA）基于分子间的相互作用，例如阴离子-π相互作用和π-π堆积，这可以通过明智地设计具有与生物大分子货物[质粒脱氧核糖核酸（DNA）相似的重复单元的聚合物小体来实现）和核糖核酸（RNA）]。根据这两个原理，聚（环氧乙烷）₄₅ - b-聚（（α-（肉桂酰氧基甲基）-1,2,3-三唑）己内酯）₉₀（PEO ₄₅ - b -PCTCL ₉₀）制备嵌段共聚物和由在水中的聚合物直接分散的自组装成聚合物囊泡。这种方法允许同时进行聚合物自组装和血红蛋白（79％），质粒DNA（75％）和RNA（85％）的超高生物大分子负载效率。透射电子显微镜和分子动力学计算机模拟证实了负责这些高负载效率的AIA和AEA原理。而且，这种新颖的聚合物囊泡具有可生物降解的膜，该膜具有可光交联的基团。这解决了长期存在的平衡电稳定性和生物降解性的问题。最后，我们展示了PEO ₄₅的生物医学潜力-b -PCTCL ₉₀聚合物小体。载有不同大小的绿色荧光蛋白编码质粒的聚合物囊泡可有效转染到HepG2细胞中，而不会干扰基因表达。总体而言，我们提出了设计具有超高负载能力的蛋白质和核酸载体的两个原则，并为开发具有可调节的生物降解性的非阳离子载体提供了启示。

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Two Principles for Polymersomes with Ultrahigh Biomacromolecular Loading Efficiencies: Acid-Induced Adsorption and Affinity-Enhanced Attraction

Herein, two novel principles are proposed for the judicious design of polymersomes with ultrahigh loading efficiencies for various biomacromolecules: (1) acid-induced adsorption (AIA) for proteins and (2) affinity-enhanced attraction (AEA) for nucleic acids. The former principle (AIA) is assisted by the triazole group within the polymersome membrane. The latter principle (AEA) is based on intermolecular interactions, such as the anion−π interaction and π–π stacking, which can be achieved by the judicious design of polymersomes with structurally similar repeat units as the biomacromolecular cargo [plasmid deoxyribonucleic acid (DNA) and ribonucleic acid (RNA)]. According to these two principles, a poly(ethylene oxide)₄₅-b-poly((α-(cinnamoyloxymethyl)-1,2,3-triazol)caprolactone)₉₀ (PEO₄₅-b-PCTCL₉₀) block copolymer was prepared and self-assembled into polymersomes by directly dispersing the polymer in water. This approach allowed simultaneous polymer self-assembly and ultrahigh biomacromolecular loading efficiencies for hemoglobin (79%), plasmid DNA (75%), and RNA (85%). The AIA and AEA principles, responsible for these high loading efficiencies, were confirmed by transmission electron microscopy and molecular dynamics computer simulations. Moreover, this novel polymersome has a biodegradable membrane with photocross-linkable groups; this solves a long-standing problem in balancing electrosteric stability and biodegradability. Finally, we demonstrated the biomedical potential of the PEO₄₅-b-PCTCL₉₀ polymersome. Polymersomes loaded with green fluorescent protein-encoded plasmid of different sizes were efficiently transfected into HepG2 cells without interfering the gene expression. Overall, we propose two principles for designing protein and nucleic acid vectors with ultrahigh loading capability and shed light on developing noncationic vectors with tunable biodegradability.

更新日期：2020-05-13

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