Self-Assembly of Amphiphilic Homopolymers Bearing Ferrocene and Carboxyl Functionalities: Effect of Polymer Concentration, β-Cyclodextrin, and Length of Alkyl Linker

Feng, Chuanqi; Lu, Guolin; Li, Yongjun; Huang, Xiaoyu

doi:10.1021/la402335d

Cited by 56 publications

(53 citation statements)

References 68 publications

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“…Hydrodynamic diameter ( D h ) of these micelles obtained from dynamic light scattering (DLS) were 181, 166, 324, and 307 nm for copolymer 4a , 4b , 4c , and 4d , respectively, which were all higher than those obtained from TEM due to the hydration effect. However, most of micelles were much larger than the theoretical length of triblock copolymer, which inferred that large compound micelles, rather than common spherical micelles, were formed5859. For these large compound micelles in the current case, micellar structure can be deemed that hydrophilic PEG and PMAA segments formed the corona of micelles and the core was consisted of numerous reverse micelles with islands of PEG and PMAA segments in continuous phase of hydrophobic PBPFCBPMA segments according to previous literatures2958.…”

Section: Resultssupporting

confidence: 55%

Perfluorocyclobutyl Aryl Ether-Based ABC Amphiphilic Triblock Copolymer

Yao

et al. 2016

Sci Rep

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A series of fluorine-containing amphiphilic ABC triblock copolymers comprising hydrophilic poly(ethylene glycol) (PEG) and poly(methacrylic acid) (PMAA), and hydrophobic poly(p-(2-(4-biphenyl)perfluorocyclobutoxy)phenyl methacrylate) (PBPFCBPMA) segments were synthesized by successive atom transfer radical polymerization (ATRP). First, PEG-Br macroinitiators bearing one terminal ATRP initiating group were prepared by chain-end modification of monohydroxy-terminated PEG via esterification reaction. PEG-b-PBPFCBPMA-Br diblock copolymers were then synthesized via ATRP of BPFCBPMA monomer initiated by PEG-Br macroinitiator. ATRP polymerization of tert-butyl methacrylate (tBMA) was directly initiated by PEG-b-PBPFCBPMA-Br to provide PEG-b-PBPFCBPMA-b-PtBMA triblock copolymers with relatively narrow molecular weight distributions (Mw/Mn ≤ 1.43). The pendant tert-butyoxycarbonyls were hydrolyzed to carboxyls in acidic environment without affecting other functional groups for affording PEG-b-PBPFCBPMA-b-PMAA amphiphilic triblock copolymers. The critical micelle concentrations (cmc) were determined by fluorescence spectroscopy using N-phenyl-1-naphthylamine as probe and the self-assembly behavior in aqueous media were investigated by transmission electron microscopy. Large compound micelles and bowl-shaped micelles were formed in neutral aqueous solution. Interestingly, large compound micelles formed by triblock copolymers can separately or simultaneously encapsulate hydrophilic Rhodamine 6G and hydrophobic pyrene agents.

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Section: Resultssupporting

confidence: 55%

Perfluorocyclobutyl Aryl Ether-Based ABC Amphiphilic Triblock Copolymer

Yao

et al. 2016

Sci Rep

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“…Amphiphilic block copolymers are well‐known systems to undergo self‐assembly in solvents to form spherical micelles and several other morphologies . Thus, metallocene‐containing amphiphilic block‐ or homopolymers exhibit interesting self‐assembly behavior . In comparison with the above‐mentioned examples, micellization behavior of statistical copolymers has only been investigated in selected studies .…”

Section: Resultsmentioning

confidence: 99%

Redox‐Switchable Supramolecular Graft Polymer Formation via Ferrocene–Cyclodextrin Assembly

Szillat

Schmidt

Hubert

et al. 2014

Macromol. Rapid Commun.

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The redox switchable formation of very well-defined supramolecular graft polymers in aqueous solution driven by host-guest interactions between ferrocene (Fc) and cyclodextrin (CD) is presented. The Fc-containing acrylic backbone copolymer (PDMA-stat-Fc) is prepared via reversible addition-fragmentation chain transfer (RAFT) copolymerization of N,N-dimethyl-acrylamide (DMA) and the novel monomer N-(ferrocenoylmethyl)acrylamide (NFMA). Via the RAFT process, copolymers containing variable Fc ratios (5-10 mol%) are prepared, affording polymers of molecular masses of close to 11,000 g mol(-1) and molar mass dispersities (Đ) of 1.2. The β-cyclodextrin (β-CD) containing building block is synthesized via RAFT-polymerization, too, in order to afford a polymer with well-defined molecular mass and low dispersity (Mn = 10 300 g mol(-1) , Đ = 1.1), employing a propargyl-functionalized chain transfer agent for the polymerization of N,N-diethylacrylamide (DEA). The polymerization product is subsequently terminated with β-CD via the regiospecific copper (I)-catalyzed 1,3-cycloaddition (PDEA-βCD). Host-guest interactions between Fc and CD lead to the formation of supramolecular graft-polymers, verified via nuclear Overhauser enhancement spectroscopy (NOESY). Importantly, their redox-responsive character is clearly confirmed via cyclic voltammetry (CV). The self-assembly of the statistical Fc-containing lateral polymer chain in aqueous solution leads to mono- and multi-core micelle-aggregates evidenced via TEM. Only diffused cloud-like, non-spherical nanostructures are observed after addition of PDEA-βCD (TEM).

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“…By changing the solvent, the long alkyl chains could bend to form reverse micelle-type assemblies ( Fig. 34 The ferrocenecontaining monomers consisted of both ferrocene and carboxylic acid formed by sequential hydrolysis. The chains fold upon increasing their lengths.…”

Section: ''Monomer-induced'' Methodsmentioning

confidence: 99%

Self-assemblies of amphiphilic homopolymers: synthesis, morphology studies and biomedical applications

et al. 2015

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The need for a simplified access to supramolecular assemblies with enhanced tenability has led to the development of amphiphilic homopolymers (APHPs). This feature article highlights recent advances and future trends in APHP design, self-assembly, and biomedical applications. APHP self-assemblies are prepared by two different routes: the "monomer-induced" method, which polymerizes functional amphiphilic monomers into micelles and inverse micelles, and the "hydrophobic-group-induced" method, which uses the non-covalent interaction provided by large hydrophobic endgroups. Special emphasis is paid to unimolecular polymeric micelles (UPMs) which are formed from core-shell APHPs and which consist of a hydrophobic/hydrophilic core coated with a polymer shell. The self-assembled supramolecular structures hold promise for various biomedical fields, including living cell transport, fluorescence labelling, protein sensing and extraction, DNA detection, and drug loading and release.

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Self-Assembly of Amphiphilic Homopolymers Bearing Ferrocene and Carboxyl Functionalities: Effect of Polymer Concentration, β-Cyclodextrin, and Length of Alkyl Linker

Cited by 56 publications

References 68 publications

Perfluorocyclobutyl Aryl Ether-Based ABC Amphiphilic Triblock Copolymer

Perfluorocyclobutyl Aryl Ether-Based ABC Amphiphilic Triblock Copolymer

Redox‐Switchable Supramolecular Graft Polymer Formation via Ferrocene–Cyclodextrin Assembly

Self-assemblies of amphiphilic homopolymers: synthesis, morphology studies and biomedical applications

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