title: Systematic design and application of unimolecular star-like block copolymer micelles: a coarse-grained simulation study.
abstract: Unimolecular polymeric micelles have several features, such as thermodynamic stability, small particle size, biocompatibility, and the ability to internalize hydrophobic molecules. These micelles have recently attracted significant attention in various applications, such as nano-reactors, catalysis, and drug delivery. However, few attempts have explored the formation mechanisms and conditions of unimolecular micelles due to limited experimental techniques. In this study, a unimolecular micelle system formed from β-cyclodextrin-graft-{poly(lactide)-block-poly(2-(dimethylamino) ethyl multimethacrylate)-block-poly[oligo (2-ethyl-2-oxazoline) methacrylate]} β-CD-g-(PLA-b-PDMAEMA-b-PEtOxMA) star-like block copolymers in aqueous media was investigated by dissipative particle dynamics (DPD) to explore the formation process of unimolecular micelles. The simulation results showed that using longer hydrophobic or pH-sensitive chains, shorter hydrophilic backbones, smaller hydrophilic side chain grafting density, and fewer polymer arms resulted in micellar aggregation. Furthermore, this unimolecular polymeric micelle could be used for encapsulating gold nanoparticles, whose mesoscopic structure was also explored. The gold nanoparticles tended to distribute in the middle layer formed by PDMAEMA, and the unimolecular micelles were capable of impeding gold nanoparticle aggregation. This study could help understand the formation mechanism of unimolecular micelles formed from star-like block copolymers in dilute solutions and offer a theoretical guide to the design and preparation of promising unimolecular polymeric micelles with targeting properties.
authors.affiliation: School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, P. R. China. celjzh@scut.edu.cn.
authors.forename: Xiaofang
authors.initials: X
authors.lastname: Zhang
authors.affiliation: School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, P. R. China. celjzh@scut.edu.cn.
authors.forename: Wenjing
authors.initials: W
authors.lastname: Lin
authors.affiliation: School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, P. R. China. celjzh@scut.edu.cn.
authors.forename: Liyang
authors.initials: L
authors.lastname: Wen
authors.affiliation: School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, P. R. China. celjzh@scut.edu.cn.
authors.forename: Na
authors.initials: N
authors.lastname: Yao
authors.affiliation: School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, P. R. China. celjzh@scut.edu.cn.
authors.forename: Shuyu
authors.initials: S
authors.lastname: Nie
authors.affiliation: School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, P. R. China. celjzh@scut.edu.cn.
authors.forename: Lijuan
authors.initials: L
authors.lastname: Zhang