Journal
COLLOIDS AND SURFACES B-BIOINTERFACES
Volume 169, Issue -, Pages 107-117Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.colsurfb.2018.05.004
Keywords
SARA ATRP; Brush-like block copolymers; Gene delivery
Funding
- MATIS - Materiais e Tecnologias Industriais Sustentaveis [CENTRO-01-0145-FEDER-000014]
- FCT-MCTES [PTDC/CTMPOL/6138/2014, CMUP-ERI/TIC/0021/2014]
- FEDER funds through the POCI - COMPETE 2020 - Operational Programme Competitiveness and Internationalization in Axis I - Strengthening research, technological development and innovation [POCI-01-0145-FEDER-007491]
- National Funds by FCT - Foundation for Science and Technology [UID/Multi/00709/2013]
- FEDER - European Regional Development Fund through the COMPETE Programme (Operational Programme for competitiveness)
- National Funds through FCT - Fundacao para a Ciencia e a Tecnologia (Portuguese Foundation for Science and Technology) [REEQ/481/QUI/2006, RECI/QEQ-QFI/0168/2012, CENTRO-07-CT62-FEDER-002012]
- Rede Nacional de Ressonancia Magnetica Nuclear (RNRMN)
- [SFRH/BD/102284/2014]
- Fundação para a Ciência e a Tecnologia [SFRH/BD/102284/2014, CMUP-ERI/TIC/0021/2014] Funding Source: FCT
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Well-defined oligo(ethylene glycol) methyl ether methacrylate (OEOMA) based block copolymers with cationic segments composed by N,N-(dimethylamino) ethyl methacrylate (DMAEMA) and/or 2-(diisopropylamino) ethyl methacrylate (DPA) were developed under biorelevant reaction conditions. These brush-type copolymers were synthesized through supplemental activator and reducing agent (SARA) atom transfer radical polymerization (ATRP) using sodium dithionite as SARA agent. The synthesis was carried out using an eco-friendly solvent mixture, very low copper catalyst concentration, and mild reaction conditions. The structure of the block copolymers was characterized by size exclusion chromatography (SEC) analysis and H-1 nuclear magnetic resonance (NMR) spectroscopy. The pH-dependent protonation of these copolymers enables the efficient complexation with plasmid DNA (pDNA), yielding polyplexes with sizes ranging from 200 up to 700 nm, depending on the molecular weight of the copolymers, composition and concentration used. Agarose gel electrophoresis confirmed the successful pDNA encapsulation. No cytotoxicity effect was observed, even for N/P ratios higher than 50, for human fibroblasts and cervical cancer cell lines cells. The in vitro cellular uptake experiments demonstrated that the pDNA-loaded block copolymers were efficiently delivered into nucleus of cervical cancer cells. The polymerization approach, the unique structure of the block copolymers and the efficient DNA encapsulation presented can open new avenues for development of efficient tailor made gene delivery systems under biorelevant conditions. (C) 2018 Elsevier B.V. All rights reserved.
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