Self-Organization of Mobile, Polyelectrolytic Dendrons on Stable, Amphiphile-Based Spherical Surfaces
Self-Organization of Mobile, Polyelectrolytic Dendrons on Stable, Amphiphile-Based Spherical Surfaces
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稳定的基于两亲物的球表面上移动聚电解树枝的自组织
DOI：
10.1021/acs.langmuir.2c03386
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发表时间：
2023
期刊：
影响因子：
3.9
通讯作者：
Dutt, Meenakshi
中科院分区：
文献类型：
--
作者：
Banerjee, Akash;Dutt, Meenakshi
带有移动的亲溶剂链的球面是普遍存在的。这些系统在自然界中以携带碳水化合物链或聚糖的生物细胞的形式存在，或在药物递送系统如携带聚乙二醇链并携带治疗分子的囊泡中存在。球表面上的链的自组织决定了后者的稳定性和功能性，并且由关键因素如链间、链-表面相互作用、排除体积、链的浓度和外部环境决定。这项研究开发了一个基本的理解，这些因素如何控制组织的移动的，亲溶剂链，同时保持稳定的球形表面。为此，该研究的重点是组织上的二棕榈酰磷脂酰胆碱为基础的囊泡的表面上的聚酰胺胺树突。排除的链和外部环境的体积，分别通过树枝化生成和pH值控制。对于酸性和碱性pH环境，树枝化延伸远离表面。因此，囊泡能够在其表面上容纳显著更高浓度的树突而不破裂。对于酸性pH，树枝化基元改变其构象以避免相互啮合。然而，对于碱性pH，由于排除体积效应，树枝化基元仅在极高浓度下改变其构象。这些构象的变化是由于质子化的树枝状残基的数量不同的pH值的函数。从这项研究的结果将推进细胞生物学，生物医学和制药的不同的子学科。
Spherical surfaces bearing mobile, solvophilic chains are ubiquitous. These systems are found in nature in the form of biological cells bearing carbohydrate chains, or glycans, or in drug delivery systems such as vesicles bearing polyethylene glycol chains and carrying therapeutic molecules. The self-organization of the chains on the spherical surface dictates the stability and functionality of the latter and is determined by key factors such as the interchain, chain–surface interactions, excluded volume, concentration of the chains, and external environment. This study develops a fundamental understanding of how these factors control the organization of mobile, solvophilic chains while preserving the stability of the spherical surface. To that end, the study focuses on the organization of polyamidoamine dendrons on the surface of a dipalmitoylphosphatidylcholine-based vesicle. The excluded volume of the chains and the external environment are, respectively, controlled via the dendron generation and the pH. For acidic and basic pH environments, the dendrons are extended away from the surface. As a consequence, the vesicles are able to accommodate significantly higher concentration of dendrons on their surface without rupturing. For acidic pH, the dendrons change their conformation to avoid intermeshing. However for basic pH, the dendrons only change their conformation at extremely high concentrations due to excluded volume effects. These conformational changes are attributed to the number of protonated dendron residues that vary as a function of pH. The results from this study will advance diverse subdisciplines within cell biology, biomedicine, and pharmaceuticals.