Multilayer onion‐like vesicles self‐assembled from amphiphilic hyperbranched multiarm copolymers via simulation

Abstract

Multilayer onion‐like vesicles are valuable in cell mimics and biomedicine fields. However, as an excellent self‐assembly precursor, the formation of multilayer onion‐like vesicles by the self‐assembly of hyperbranched multiarm copolymers (HMCs) were not reported due to the complex self‐assembly dynamics. In this article, the self‐assembly behavior of multilayer onion‐like vesicles from HMCs was systematically investigated using dissipative particle dynamics simulation. The formation conditions for different kinds of vesicles were disclosed through the construction of the morphological phase diagram. Moreover, the formation mechanisms of the onion‐like vesicles with different layers were revealed. We observed that it is the fusion mechanism in low concentrations and the molecular rearrangement mechanism in high concentrations. For low concentration, the law between the number of the membrane layers and the morphology of the aggregates in the fusion process was disclosed. Meanwhile, the membrane of the onion‐like vesicles self‐assembled from HMCs is monolayer structure and the thickness of each layer is decreased in sequence from inside to outside. The current observations have important guiding significance for its application in drug delivery systems.

Dissipative Particle Dynamics Simulation: A Review on Investigating Mesoscale Properties of Polymer Systems

“…The self‐assembly process of amphiphilic, hyperbranched, multi‐arm copolymers (HMCs) has also been simulated using DPD. [ 60–65 ] The degree of branching greatly influences the self‐assembled structure of HMCs. With the aid of DPD simulations, the study of different branching conditions revealed the self‐assembly mechanism and the kinetic formation process.…”

“…The self‐assembly behavior of multilayer onion‐like vesicles has been systematically investigated as well. [ 62 ] In this study, different numbers of layers were obtained by adjusting the polymer concentration. The results revealed that the onion‐like vesicles have a monolayered structure.…”

“…In addition to the above application fields, DPD is also used to study the degree of the cell damage caused by residual drugs [ 92–101 ] and successfully predict the self‐assembly behavior of drug carriers. [ 62,102–111 ]…”

Molecular Modelling Guided Modulation of Molecular Shape and Charge for Design of Smart Self-Assembled Polymeric Drug Transporters

“…They also found that the size of dendrimersomes will not increase through mutual fusion once the well-defined onion-like structure is formed, unlike numerous lipidsomes and polymersomes that can spontaneously coalesce. Future work combining their hard chain model with the previous reports using flexible chain models [ 144 , 147 , 148 , 149 , 151 , 152 ] could more fully characterize and predict the potential of dendrimersomes for applications in drug and gene delivery.…”

Hydrophobe Containing Polypeptoids Complex with Lipids and Induce Fusogenesis of Lipid Vesicles

“…Recent interesting work describes the use of dendrimersomes or multilamellar vesicles formed using amphiphilic Janus dendrimers by injecting THF solutions of the dendrimer into water or a buffer. 11 , 12 These are multistep synthetic processes involving the use of organic solvents, and their nontoxicity remains to be determined. Other recent examples include the use of rodlike oligofluorenes in a acetonitrile–water mixed solvent.…”