Block Sequence Effects on the Self-Assembly Behaviors of Polypeptide-Based Penta-Block Copolymer Hydrogels

Ke Hsin Wang, Chung Hao Liu, Dun Heng Tan, Mu Ping Nieh, Wei Fang Su

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Peptide-based hydrogels have great potential for applications in tissue engineering, drug delivery, and so on. We systematically synthesize, characterize, and investigate the self-assembly behaviors of a series of polypeptide-based penta-block copolymers by varying block sequences and lengths. The copolymers contain hydrophobic blocks of poly(γ-benzyl-l-glutamate) (PBG, Bx) and two kinds of hydrophilic blocks, poly(l-lysine) (PLL, Ky) and poly(ethylene glycol) (PEG, EG34), where x and y are the number of repeating units of each block, where PBG and PLL blocks have unique functions for nerve regeneration and cell adhesion. It shows that a sufficient length of the middle hydrophilic segment capped with hydrophobic end PBG blocks is required. They first self-assemble into flower-like micelles and sequentially form transparent hydrogels (as low as 2.3 wt %) with increased polymer concentration. The hydrogels contain a microscale porous structure, a desired property for tissue engineering to facilitate the access of nutrient flow for cell growth and drug delivery systems with high efficiency of drug storage. We hypothesize that the structure of Bx-Ky-EG34-Ky-Bx agglomerates is beyond micron size (transparent), while that of Ky-Bx-EG34-Bx-Ky is on the submicron scale (opaque). We establish a working strategy to synthesize a polypeptide-based block copolymer with a wide window of sol-gel transition. The study offers insight into rational polypeptide hydrogel design with specific morphology, exploring the novel materials as potential candidates for neural tissue engineering.

Original languageEnglish
Pages (from-to)6674-6686
Number of pages13
JournalACS Applied Materials and Interfaces
Volume16
Issue number5
DOIs
StatePublished - Feb 7 2024
Externally publishedYes

Funding

The authors thank the National Synchrotron Radiation Research Center (NSRRC) of Taiwan for providing SAXS facility. Financial support from the National Science and Technology Council of Taiwan (grant number: MOST 111-2221-E-002-029) is also acknowledged.

Keywords

  • block copolymer
  • hydrogel
  • micelle
  • peptide
  • self-assembly
  • small-angle X-ray scattering

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