Hydrogels from amphiphilic star block copolypeptides

Murphy, Ray; Borase, Tushar; Payne, Christina; O’Dwyer, Joanne; Cryan, Sally‐Ann; Heise, Andreas

doi:10.1039/c6ra01190j

Cited by 30 publications

(22 citation statements)

References 45 publications

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“…Sharp absorbance peaks were recorded at 1770 cm −1 for the amide and carbonyl stretches of L‐alanine‐NCA, respectively. The presence of amide I and amide II stretches at 1637 and 1540 cm −1 , respectively, indicates the formation of poly(peptide) amide bonds 23–26 …”

Section: Resultsmentioning

confidence: 99%

“…The co-occurrence of random coil, β-sheet, and β-turn configurations seems conceivable considering the complex polypeptide architecture. 24 The secondary structure of the mPEG-PA in aqueous solvent shifted from β-sheets to α-helices as the mPEG molecular weight M n increased from 2000 to 5000 and PA molecular weight M n decreased from 2500 to 1500 (Figure 4). 27 21 .…”

Section: Secondary Structures In Bcpmentioning

confidence: 99%

“…The presence of amide I and amide II stretches at 1637 and 1540 cm −1 , respectively, indicates the formation of poly(peptide) amide bonds. [23][24][25][26] From FTIR analysis, mPEG-PA display some characteristics of poly(peptide) structures due to the successful synthesis. The complex structure of amide-based functional groups such as amide I and amide II stretches dominate the film structure at longer PA chain length.…”

Section: Synthesis and Characterization Of Mpeg-pa Hydrogelsmentioning

confidence: 99%

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Self‐assembly and sol‐to‐gel transition of thermosensitive methoxy‐polyethylene glycol‐polyalanine block copolymer hydrogels

Chu

2020

J of Applied Polymer Sci

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Certain amphiphilic polymers can self-assemble to form various structures, such as micelles and hydrogels in aqueous medium, depending on the concentration or temperature. These different structures have found many applications in biomedical and material processing fields. The assembly processes of the polypeptide-containing diblock copolymer, methoxy poly(ethylene glycol)block-poly(L-alanine) (mPEG-PA), was studied to elucidate the relationship between different structures with parameters such as chain lengths (volume fraction) of the two blocks, molecular weights, medium polarity, temperature, and concentration. Gelation mechanism was especially focused in the study. Various solution-cast morphologies observed by scanning electron microscopy (SEM) imaging including cylinders and micelles aggregates can be obtained by using solvents with different polarity for casting with simply tuning the chain lengths. The sol-to-gel transition mechanism can be best explained by phase separation between polymer-rich and water-rich phases. It might be spinodal decomposition process to cause the phase separation. Furthermore, the branch and flack structures can be observed due to phase separation mechanism and different chain lengths by SEM images. This result offers new insights into behavior of mPEG-PA system, enabling more controlled manipulation to various applications.

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Section: Resultsmentioning

confidence: 99%

Section: Secondary Structures In Bcpmentioning

confidence: 99%

Section: Synthesis and Characterization Of Mpeg-pa Hydrogelsmentioning

confidence: 99%

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Self‐assembly and sol‐to‐gel transition of thermosensitive methoxy‐polyethylene glycol‐polyalanine block copolymer hydrogels

Chu

2020

J of Applied Polymer Sci

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“…Native amino acids have been utilized as polymeric blocks in these supramolecular gelators, contributing to materials with tailored mechanical properties due to control of conformational assemblies . The physical bonding contributing to gelation usually emanates from the polypeptide chain composition via electrostatic interactions, hydrophobic interactions, hydrogen bonding, π–π stacking, and van der Waals forces . The resulting hydrogels possess relatively moderate mechanical strength in addition to unique properties as a consequence of their reversible non‐covalent bonding character.…”

Section: Introductionmentioning

confidence: 99%

Gelating polypeptide matrices based on the difunctional N‐carboxyanhydride diaminopimelic acid cross‐linker

Murphy

Bobbi

Oliveira

et al. 2019

J. Polym. Sci. Part A: Polym. Chem.

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This work reports the synthesis of a new difunctional N-carboxyanhydride (NCA) monomer, namely diaminopimelic acid (DAP), and its use in the one-pot preparation of an organogelating copolypeptide. The organogel is formed in situ through ring-opening polymerization (ROP) of DAP NCA from helical poly(ε-carbobenzyloxy-L-lysine) (PZLL) blocks in a mixture of dimethylformamide/chloroform. Gelation occurs by immobilizing the solvent through core crosslinking and is stabilized through physical intermolecular conformations. After removal of the carbobenzyloxy (cbz or Z) protecting groups, the network remains intact in exceedingly high aqueous concentrations (99.5%). FTIR is used to characterize the secondary structure, revealing the conformational arrangements that contributed to these stabilized gel networks with their relative mechanical properties determined via real-time rheological assays. DAP core crosslink of the random coil forming polypeptoid poly(sarcosine) (PSar) is also resulting in networks but is devoid of any stabilized physical interactions, thus yielding significantly weaker gels as a result.

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“…[12][13][14][15] We and others have also found that use of multiblock and star copolymer architectures can enhance hydrogel properties in hydrophobically assembled copolypeptide systems. [16][17][18][19] However, these amphiphilic materials can be difficult to formulate, especially at higher concentrations, and the reported systems are not cell compatible. 18,20 Here, we sought to develop PIC multiblock copolypeptide hydrogels that could overcome these issues and allow the preparation of hydrogels with a broad range of tunable properties.…”

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confidence: 99%

Self-Healing Multiblock Copolypeptide Hydrogels via Polyion Complexation

Sun

Deming

2019

ACS Macro Lett.

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Diblock, triblock and pentablock copolypeptides were designed and prepared for formation of polyion complex hydrogels in aqueous media. Increasing the number of block segments was found to allow formation of hydrogels with substantially enhanced stiffness at equivalent concentrations. Use of similar length ionic segments also allowed mixing of different block architectures to fine tune hydrogel properties. The pentablock hydrogels possess a promising combination of high stiffness, rapid self-healing properties, and cell compatible surface chemistry that makes them promising candidates for applications requiring injectable or printable hydrogel scaffolds. Polyion complex (PIC) assembly of dual hydrophilic block copolymers containing non-ionic and oppositely charged ionic segments has been developed as a facile method to prepare a diverse array of micelles, vesicles, and hydrogels in aqueous media. 1-3 Due to the high water solubility of precursors, PIC formation allows the preparation of supramolecular assemblies at high concentrations via simple mixing, and does not require the use of either heating or cosolvents. These assemblies are experiencing extensive development in applications, including as carriers for therapeutic molecules and as scaffolds for cell culture and tissue repair. 1-5 We recently reported the design of PIC diblock copolypeptide hydrogels

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Hydrogels from amphiphilic star block copolypeptides

Abstract: Star-shaped amphiphilic block copolymers form hydrogels as opposed to their linear counterparts.

Cited by 30 publications

References 45 publications

Self‐assembly and sol‐to‐gel transition of thermosensitive methoxy‐polyethylene glycol‐polyalanine block copolymer hydrogels

Self‐assembly and sol‐to‐gel transition of thermosensitive methoxy‐polyethylene glycol‐polyalanine block copolymer hydrogels

Gelating polypeptide matrices based on the difunctional N‐carboxyanhydride diaminopimelic acid cross‐linker

Self-Healing Multiblock Copolypeptide Hydrogels via Polyion Complexation

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