Thermoreversible Hydrogels from RAFT-Synthesized BAB Triblock Copolymers: Steps toward Biomimetic Matrices for Tissue Regeneration

Kirkland, Stacey E.; Hensarling, Ryan M.; McConaughy, Shawn D.; Guo, Yan‐Lin; Jarrett, William L.; McCormick, Charles L.

doi:10.1021/bm700968t

Cited by 129 publications

(140 citation statements)

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“…Liu and coworkers also reported schizophrenic assembly behavior of a dual responsive diblock copolymer, poly(N-isopropyl acrylamide) 65 -b-poly(LGA) 110 (PNIPAM 65 -b-PLGA 110 ). 76 At pH below 4 and at 25 C, they report spherical micelles formation with PNIPAM as the corona and the hydrophobic PLGA as the core.…”

Section: Assembly and Responsiveness Of Peptide-based Diblock Copolymersmentioning

confidence: 99%

“…105,106 Assembly Behavior of BAB Linear Triblock Copolymers with a Responsive Polypeptide Inner Block The aqueous self-assembly behavior of linear triblock BAB copolymers has been evaluated widely for synthetic coilcoil-coil type systems. [107][108][109][110][111] These type of systems are reported to aggregate into sunflower micelles, enabled by molecular bending of a flexible middle block, in dilute solution. 108,111 At higher concentrations, these systems often form network structures from the association of corona chains between micelles resulting in hydrogelation.…”

Section: Synthetic Techniques For Polypeptide-based Copolymers With Tmentioning

confidence: 99%

“…108,111 At higher concentrations, these systems often form network structures from the association of corona chains between micelles resulting in hydrogelation. 107,109,110,112,113 A few studies have been devoted to self-assembly of coil-rod-coil BAB triblock copolymers containing a functionalized, hydrophilic gold nanorod center FEATURE ARTICLE block and hydrophobic coil outer blocks. [114][115][116] This category of amphiphilic molecules exhibited self-assembly into ''doughnut-like" supramolecular barrels (similar to toroid micelles), as a result of stiffness from the center block.…”

Section: Synthetic Techniques For Polypeptide-based Copolymers With Tmentioning

confidence: 99%

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Self‐assembly and responsiveness of polypeptide‐based block copolymers: How “Smart” behavior and topological complexity yield unique assembly in aqueous media

Ray¹,

Johnson²,

Savin³

2013

J Polym Sci B Polym Phys

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Polypeptide-based amphiphilic block copolymers are an attractive class of materials given their ability to form welldefined aqueous nanoassemblies that respond to external stimulus through secondary structure transitions. This report will highlight recent literature in the area of polypeptide-based block copolymer self-assembly, with the major focus being on how the responsive nature and structural complexity of the polypeptide blocks can be incorporated into systems with complex topologies such as ABA/BAB/ABC triblock copolymers, AB 2 and A 2 B star copolymers, and miktoarm l-ABC star terpolymers. In particular, the role of interfacial curvature changes and how they result in morphology transitions will be discussed. The 'smart' assembly properties of peptides in complex block copolymer topologies can lead to enhanced responsiveness, morphological complexity, and unique morphological transitions with varying solution conditions. V C 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2013, 51, 508-523 KEYWORDS: amphiphiles; biomimetic; block copolymers; selfassembly INTRODUCTION Amphiphilic block copolymers are able to self-assemble into well-defined nanostructures in aqueous solution. [1][2][3][4][5] The equilibrium morphology and aggregation number of diblock copolymer assemblies is primarily determined by the balance of three energetic factors: (1) interfacial tension, (2) corona chain crowding, and (3) core chain stretching. The balance of these three factors dictates an equilibrium curvature for the aggregate. 6-8 Typically, solution morphologies formed by amphiphilic block copolymers follow a trend of increasing interfacial curvature. As the hydrophilic fraction is increased in the copolymer, vesicles, cylindrical micelles, and spherical micelles (in the order of increasing interfacial curvature,) are the most common morphologies (Figure 1). 5,9,10 Physically, this is explained as a balance between entropic freedom of the hydrophilic coronal chains and shielding of the hydrophobic blocks from the aqueous solution; as the hydrophilic fraction increases, the chains are more able to effectively stabilize these assemblies without close-packing, and the free energy of the system is lowered when the coronal chains are provided more entropic freedom/mobility through increased curvature.

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Section: Assembly and Responsiveness Of Peptide-based Diblock Copolymersmentioning

confidence: 99%

Section: Synthetic Techniques For Polypeptide-based Copolymers With Tmentioning

confidence: 99%

Section: Synthetic Techniques For Polypeptide-based Copolymers With Tmentioning

confidence: 99%

See 1 more Smart Citation

Self‐assembly and responsiveness of polypeptide‐based block copolymers: How “Smart” behavior and topological complexity yield unique assembly in aqueous media

Ray¹,

Johnson²,

Savin³

2013

J Polym Sci B Polym Phys

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“…In the case of bis-RAFT agents sequential polymerization of two monomers will yield a triblock. [269] BA [270] MA [270] NIPAM [269,[271][272][273] 420 [274] BA [281] DA [281] St [71,275] 2VP [276] NVP [103] NIPAM/274 [153] DEHEA [280] MA [281] TMAPMA/PEGMA/NIPAM [277] (PEGMA/320) [165] tBA [280] BA/AA [279] (PEGMA/344) [165] 331 [159] AEMA/325/328 [278] DEHEA-b-ODA [280] DMAM-b-331 [159] DMAM-b-331-b-NIPAM [159] DEHEA-b-tBA [280] NIPAM-b-DMAM [272] 2VP-b-EA [276] tBA-b-DEHEA [280] AEME/328/342 [278] 105 [282] [282] PEGA-b-St [282] 106 [188] [188] EHA-b-MA [188] S S S…”

Section: *mentioning

confidence: 99%

“…Physically crosslinked hydrogel networks can be prepared by the assembly of RAFT-synthesized triblock copolymers. [86,272,[546][547][548] The structures can be tuned to absorb either hydrophilic or hydrophobic substrates and to swell in specific media or in response to various stimuli such as pH, temperature, ionic strength, etc. by appropriate monomer selection.…”

Section: Polymer Networkmentioning

confidence: 99%

Living Radical Polymerization by the RAFT Process - A Second Update

Moad¹,

Rizzardo²,

Thang³

2009

Aust. J. Chem.

906

720

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This paper provides a second update to the review of reversible deactivation radical polymerization achieved with thiocarbonylthio compounds (ZC(=S)SR) by a mechanism of reversible addition-fragmentation chain transfer (RAFT) that was published in June 2005 (Aust. J. Chem. 2005, 58, 379-410). The first update was published in November 2006 (Aust. J. Chem. 2006, 59, 669-692). This review cites over 500 papers that appeared during the period mid-2006 to mid-2009 covering various aspects of RAFT polymerization ranging from reagent synthesis and properties, kinetics and mechanism of polymerization, novel polymer syntheses and a diverse range of applications. Significant developments have occurred, particularly in the areas of novel RAFT agents, techniques for end-group removal and transformation, the production of micro/nanoparticles and modified surfaces, and biopolymer conjugates both for therapeutic and diagnostic applications.

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Physical Hydrogels

Tsitsilianis

2013

Encyclopedia of Polymer Science and Technology

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The present article concerns a special class of soft mater, namely physical hydrogels or self‐assembling hydrogels. The best suited polymeric building elements for the creation of temporary networks are water‐soluble segmented macromolecules bearing attractive groups, capable of developing physical bonds through intermolecular associations. The present article focuses on physical hydrogels formed by well‐defined polymers, exhibiting the triblock topology. Hydrogels organized through jamming of nonconnected micellar entities, for example, diblock copolymers and surfactants, are not included. The self‐organization of these associative polymeric species when dissolved in water results in complex fluids with intriguing rheological properties, attracting considerable interest in numerous applications as, for instance, in the fields of cosmetics, pharmaceutics, coatings, and biomedicine for tissue engineering and controlled drug delivery.

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Thermoreversible Hydrogels from RAFT-Synthesized BAB Triblock Copolymers: Steps toward Biomimetic Matrices for Tissue Regeneration

Cited by 129 publications

References 63 publications

Self‐assembly and responsiveness of polypeptide‐based block copolymers: How “Smart” behavior and topological complexity yield unique assembly in aqueous media

Self‐assembly and responsiveness of polypeptide‐based block copolymers: How “Smart” behavior and topological complexity yield unique assembly in aqueous media

Living Radical Polymerization by the RAFT Process - A Second Update

Physical Hydrogels

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