Biodegradable core-shell materials via RAFT and ROP: Characterization and comparison of hyperbranched and microgel particles

Zheng, Yu, Turner, William, Zong, Mengmeng, Irvine, Derek J., Howdle, Steven M. and Thurecht, Kristofer J. (2011) Biodegradable core-shell materials via RAFT and ROP: Characterization and comparison of hyperbranched and microgel particles. Macromolecules, 44 6: 1347-1354. doi:10.1021/ma1027092


Author Zheng, Yu
Turner, William
Zong, Mengmeng
Irvine, Derek J.
Howdle, Steven M.
Thurecht, Kristofer J.
Title Biodegradable core-shell materials via RAFT and ROP: Characterization and comparison of hyperbranched and microgel particles
Journal name Macromolecules   Check publisher's open access policy
ISSN 0024-9297
1520-5835
Publication date 2011-03-22
Sub-type Article (original research)
DOI 10.1021/ma1027092
Volume 44
Issue 6
Start page 1347
End page 1354
Total pages 8
Place of publication Washington, DC, United States
Publisher American Chemical Society
Collection year 2012
Language eng
Formatted abstract
Two methodologies for synthesizing novel, degradable, core cross-linked copolymer particles were investigated and the molecular properties of the resultant polymers were compared. The first approach was to synthesize hyperbranched poly(ε-caprolactone-co-N,N-dimethylamino-2-ethyl methacrylate (PCL-co-PDMAEMA) by combining metal-catalyzed ring-opening polymerization (ROP) of ε-caprolactone (ε-CL) and reversible addition−fragmentation chain transfer polymerization (RAFT) of N,N-dimethylamino-2-ethyl methacrylate. First, the hyperbranched core was prepared via ROP copolymerization of ε-CL and branching agent 4,4-bioxepanyl-7,7-dione (BOD). This polymerization was initiated using the hydroxyl moiety of the bifunctional initiator 4-cyano-1-hydroxypent-4-yl dithiobenzoate (ACP-RAFT) which resulted in reactive pendent RAFT groups located on the polymer chains. The hyperbranched structure was confirmed by GPC-MALLS and NMR. Subsequent chain extension of this hyperbranched macromolecule with DMAEMA using RAFT chemistry yielded water-soluble nanoparticles. The second method involved the synthesis of core-cross-linked-shell particles (CCS) by the arm-first route. Linear arms of DMAEMA were synthesized using ACP-RAFT and subsequently used as macroinitiator for the ROP of ε-CL and BOD to form a degradable microgel that was water-soluble. Once again, molecular structure was analyzed by 1H NMR, 13C NMR, and GPC and molecular size by TEM. Finally, GPC-MALLS was used to qualitatively investigate the different cross-link densities of the degradable core by the two different methodologies. Thus, we demonstrate two synthetic approaches for constructing water-soluble, degradable core−shell nanoparticles that exhibit varying degrees of cross-linking by combining RAFT and ROP.
Q-Index Code C1
Q-Index Status Confirmed Code
Institutional Status UQ

Document type: Journal Article
Sub-type: Article (original research)
Collections: Official 2012 Collection
Centre for Advanced Imaging Publications
 
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Created: Wed, 25 Jan 2012, 11:24:37 EST by Sandrine Ducrot on behalf of Centre for Advanced Imaging