Stereocomplexed 8-armed poly(ethylene glycol)-poly(lactide) star block copolymer hydrogels: Gelation mechanism, mechanical properties and degradation behavior

S.J. Buwalda, L. Calucci, C. Forte, Pieter J. Dijkstra, Jan Feijen

Research output: Contribution to journalArticleAcademicpeer-review

36 Citations (Scopus)

Abstract

Mixing aqueous poly(ethylene glycol)-poly(d-lactide) and poly(ethylene glycol)-poly(l-lactide) star block copolymer solutions resulted in the formation of stereocomplexed hydrogels within 1 min. A study towards the mechanism of the temperature dependent formation of stereocomplexes in the hydrogels using rheology and nuclear magnetic resonance experiments revealed that the formation of stereocomplexes is facilitated at higher temperatures, due to rearrangement in the micellar aggregates thereby exposing more PLA units available for stereocomplexation. The formed gels became temperature irreversible due to the presence of highly stable semi-crystalline stereocomplexed PLA domains. An enantiomeric mixture of 8-armed star block copolymers linked by an amide group between the poly(ethylene glycol) core and the poly(lactide) arms (PEG–(NHCO)–(PLA)8) yielded hydrogels with improved mechanical properties and stability at 37 °C in PBS compared to 8-armed star block copolymers linked by an ester group. The possibility to be formed in situ in combination with their robustness make PEG–(NHCO)–(PLA)8 hydrogels appealing materials for various biomedical applications.
Original languageEnglish
Pages (from-to)2809-2817
JournalPolymer
Volume53
Issue number14
DOIs
Publication statusPublished - 2012

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Hydrogels
Gelation
Polyethylene glycols
Block copolymers
Stars
Degradation
Mechanical properties
Mechanical stability
Rheology
Amides
Temperature
Esters
Gels
Nuclear magnetic resonance
poly(lactide)
Crystalline materials
Experiments

Keywords

  • METIS-288521
  • IR-81899

Cite this

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title = "Stereocomplexed 8-armed poly(ethylene glycol)-poly(lactide) star block copolymer hydrogels: Gelation mechanism, mechanical properties and degradation behavior",
abstract = "Mixing aqueous poly(ethylene glycol)-poly(d-lactide) and poly(ethylene glycol)-poly(l-lactide) star block copolymer solutions resulted in the formation of stereocomplexed hydrogels within 1 min. A study towards the mechanism of the temperature dependent formation of stereocomplexes in the hydrogels using rheology and nuclear magnetic resonance experiments revealed that the formation of stereocomplexes is facilitated at higher temperatures, due to rearrangement in the micellar aggregates thereby exposing more PLA units available for stereocomplexation. The formed gels became temperature irreversible due to the presence of highly stable semi-crystalline stereocomplexed PLA domains. An enantiomeric mixture of 8-armed star block copolymers linked by an amide group between the poly(ethylene glycol) core and the poly(lactide) arms (PEG–(NHCO)–(PLA)8) yielded hydrogels with improved mechanical properties and stability at 37 °C in PBS compared to 8-armed star block copolymers linked by an ester group. The possibility to be formed in situ in combination with their robustness make PEG–(NHCO)–(PLA)8 hydrogels appealing materials for various biomedical applications.",
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author = "S.J. Buwalda and L. Calucci and C. Forte and Dijkstra, {Pieter J.} and Jan Feijen",
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language = "English",
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Stereocomplexed 8-armed poly(ethylene glycol)-poly(lactide) star block copolymer hydrogels: Gelation mechanism, mechanical properties and degradation behavior. / Buwalda, S.J.; Calucci, L.; Forte, C.; Dijkstra, Pieter J.; Feijen, Jan.

In: Polymer, Vol. 53, No. 14, 2012, p. 2809-2817.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Stereocomplexed 8-armed poly(ethylene glycol)-poly(lactide) star block copolymer hydrogels: Gelation mechanism, mechanical properties and degradation behavior

AU - Buwalda, S.J.

AU - Calucci, L.

AU - Forte, C.

AU - Dijkstra, Pieter J.

AU - Feijen, Jan

PY - 2012

Y1 - 2012

N2 - Mixing aqueous poly(ethylene glycol)-poly(d-lactide) and poly(ethylene glycol)-poly(l-lactide) star block copolymer solutions resulted in the formation of stereocomplexed hydrogels within 1 min. A study towards the mechanism of the temperature dependent formation of stereocomplexes in the hydrogels using rheology and nuclear magnetic resonance experiments revealed that the formation of stereocomplexes is facilitated at higher temperatures, due to rearrangement in the micellar aggregates thereby exposing more PLA units available for stereocomplexation. The formed gels became temperature irreversible due to the presence of highly stable semi-crystalline stereocomplexed PLA domains. An enantiomeric mixture of 8-armed star block copolymers linked by an amide group between the poly(ethylene glycol) core and the poly(lactide) arms (PEG–(NHCO)–(PLA)8) yielded hydrogels with improved mechanical properties and stability at 37 °C in PBS compared to 8-armed star block copolymers linked by an ester group. The possibility to be formed in situ in combination with their robustness make PEG–(NHCO)–(PLA)8 hydrogels appealing materials for various biomedical applications.

AB - Mixing aqueous poly(ethylene glycol)-poly(d-lactide) and poly(ethylene glycol)-poly(l-lactide) star block copolymer solutions resulted in the formation of stereocomplexed hydrogels within 1 min. A study towards the mechanism of the temperature dependent formation of stereocomplexes in the hydrogels using rheology and nuclear magnetic resonance experiments revealed that the formation of stereocomplexes is facilitated at higher temperatures, due to rearrangement in the micellar aggregates thereby exposing more PLA units available for stereocomplexation. The formed gels became temperature irreversible due to the presence of highly stable semi-crystalline stereocomplexed PLA domains. An enantiomeric mixture of 8-armed star block copolymers linked by an amide group between the poly(ethylene glycol) core and the poly(lactide) arms (PEG–(NHCO)–(PLA)8) yielded hydrogels with improved mechanical properties and stability at 37 °C in PBS compared to 8-armed star block copolymers linked by an ester group. The possibility to be formed in situ in combination with their robustness make PEG–(NHCO)–(PLA)8 hydrogels appealing materials for various biomedical applications.

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KW - IR-81899

U2 - 10.1016/j.polymer.2012.05.006

DO - 10.1016/j.polymer.2012.05.006

M3 - Article

VL - 53

SP - 2809

EP - 2817

JO - Polymer

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SN - 0032-3861

IS - 14

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