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Polymers 2016, 8(11), 397; doi:10.3390/polym8110397

Co-Delivery of Imiquimod and Plasmid DNA via an Amphiphilic pH-Responsive Star Polymer that Forms Unimolecular Micelles in Water

1
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China
2
Department of Biomedical Engineering, University of Minnesota, Minneapolis, MN 55455, USA
3
State Key Laboratory of Medicinal Chemical Biology and Tianjin Key Laboratory of Molecular Drug Research, College of Pharmacy, Nankai University, Tianjin 300071, China
*
Authors to whom correspondence should be addressed.
Academic Editor: Raechelle D’Sa
Received: 12 October 2016 / Revised: 8 November 2016 / Accepted: 9 November 2016 / Published: 16 November 2016
(This article belongs to the Special Issue Advance of Polymers Applied to Biomedical Applications: Biointerface)
View Full-Text   |   Download PDF [11343 KB, uploaded 16 November 2016]   |  

Abstract

Dual functional unimolecular micelles based on a pH-responsive amphiphilic star polymer β-CD-(PLA-b-PDMAEMA-b-PEtOxMA)21 have been developed for the co-delivery of imiquimod and plasmid DNA to dendritic cells. The star polymer with well-defined triblock arms was synthesized by combining activator regenerated by electron-transfer atom-transfer radical polymerization with ring-opening polymerization. Dissipative particle dynamics simulation showed that core-mesophere-shell-type unimolecular micelles could be formed. Imiquimod-loaded micelles had a drug loading of 1.6 wt % and a larger average size (28 nm) than blank micelles (19 nm). The release of imiquimod in vitro was accelerated at the mildly acidic endolysosomal pH (5.0) in comparison to physiologic pH (7.4). Compared with blank micelles, a higher N:P ratio was required for imiquimod-loaded micelles to fully condense DNA into micelleplexes averaging 200–400 nm in size. In comparison to blank micelleplexes, imiquimod-loaded micelleplexes of the same N:P ratio displayed similar or slightly higher efficiency of gene transfection in a mouse dendritic cell line (DC2.4) without cytotoxicity. These results suggest that such pH-responsive unimolecular micelles formed by the well-defined amphiphilic star polymer may serve as promising nano-scale carriers for combined delivery of hydrophobic immunostimulatory drugs (such as imiquimod) and plasmid DNA with potential application in gene-based immunotherapy. View Full-Text
Keywords: co-delivery; pH-responsive; unimolecular micelles; immunotherapy co-delivery; pH-responsive; unimolecular micelles; immunotherapy
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Lin, W.; Yao, N.; Li, H.; Hanson, S.; Han, W.; Wang, C.; Zhang, L. Co-Delivery of Imiquimod and Plasmid DNA via an Amphiphilic pH-Responsive Star Polymer that Forms Unimolecular Micelles in Water. Polymers 2016, 8, 397.

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