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Redox-responsive hydrogels for tunable and 'on-demand' release of biomacromolecules

(2022) BIOCONJUGATE CHEMISTRY. 33(5). p.839-847
Author
Organization
Abstract
In recent years, stimuli-responsive degradation has emerged as a desirable design criterion for functional hydrogels to tune the release of encapsulated payload as well as ensure degradation of the gel upon completion of its function. Herein, redox-responsive hydrogels with a well-defined network structure were obtained using a highly efficient thiol-disulfide exchange reaction. In particular, gelation occurred upon combining thiol-terminated tetra-arm polyethylene glycol (PEG) polymers with linear telechelic PEG-based polymers containing pyridyl disulfide units at their chain ends. Rapid gelation proceeds with good conversions (>85%) to yield macroporous hydrogels possessing high water uptake. Furthermore, due to the presence of the disulfide linkages, the thus-obtained hydrogels can self-heal. The obtained hydrogels undergo complete degradation when exposed to environments rich in thiol-containing agents such as dithiothreitol (DTT) and L-glutathione (GSH). Also, the release profile of encapsulated protein, namely, bovine serum albumin, can be tuned by varying the molecular weight of the polymeric precursors. Additionally, it was demonstrated that complete dissolution of the hydrogel to rapidly release the encapsulated protein occurs upon treating these hydrogels with DTT. Cytotoxicity evaluation of the hydrogels and their degradation products indicated the benign nature of these hydrogels. Additionally, the cytocompatible nature of these materials was also evident from a live/dead cell viability assay. One can envision that the facile fabrication and their ability to degrade on-demand and release their payload will make these benign polymeric scaffolds attractive for various biomedical applications.
Keywords
Organic Chemistry, Pharmaceutical Science, Pharmacology, Biomedical Engineering, Bioengineering, Biotechnology, POLY(ETHYLENE GLYCOL) HYDROGELS, DELIVERY, COPOLYMERS, FUNCTIONALIZATION, DISSOLUTION, FABRICATION, NANOGELS

Citation

Please use this url to cite or link to this publication:

MLA
Kilic Boz, Ruveyda, et al. “Redox-Responsive Hydrogels for Tunable and ‘on-Demand’ Release of Biomacromolecules.” BIOCONJUGATE CHEMISTRY, vol. 33, no. 5, 2022, pp. 839–47, doi:10.1021/acs.bioconjchem.2c00094.
APA
Kilic Boz, R., Aydin, D., Kocak, S., Golba, B., Sanyal, R., & Sanyal, A. (2022). Redox-responsive hydrogels for tunable and “on-demand” release of biomacromolecules. BIOCONJUGATE CHEMISTRY, 33(5), 839–847. https://doi.org/10.1021/acs.bioconjchem.2c00094
Chicago author-date
Kilic Boz, Ruveyda, Duygu Aydin, Salli Kocak, Bianka Golba, Rana Sanyal, and Amitav Sanyal. 2022. “Redox-Responsive Hydrogels for Tunable and ‘on-Demand’ Release of Biomacromolecules.” BIOCONJUGATE CHEMISTRY 33 (5): 839–47. https://doi.org/10.1021/acs.bioconjchem.2c00094.
Chicago author-date (all authors)
Kilic Boz, Ruveyda, Duygu Aydin, Salli Kocak, Bianka Golba, Rana Sanyal, and Amitav Sanyal. 2022. “Redox-Responsive Hydrogels for Tunable and ‘on-Demand’ Release of Biomacromolecules.” BIOCONJUGATE CHEMISTRY 33 (5): 839–847. doi:10.1021/acs.bioconjchem.2c00094.
Vancouver
1.
Kilic Boz R, Aydin D, Kocak S, Golba B, Sanyal R, Sanyal A. Redox-responsive hydrogels for tunable and “on-demand” release of biomacromolecules. BIOCONJUGATE CHEMISTRY. 2022;33(5):839–47.
IEEE
[1]
R. Kilic Boz, D. Aydin, S. Kocak, B. Golba, R. Sanyal, and A. Sanyal, “Redox-responsive hydrogels for tunable and ‘on-demand’ release of biomacromolecules,” BIOCONJUGATE CHEMISTRY, vol. 33, no. 5, pp. 839–847, 2022.
@article{8750512,
  abstract     = {{In recent years, stimuli-responsive degradation has emerged as a desirable design criterion for functional hydrogels to tune the release of encapsulated payload as well as ensure degradation of the gel upon completion of its function. Herein, redox-responsive hydrogels with a well-defined network structure were obtained using a highly efficient thiol-disulfide exchange reaction. In particular, gelation occurred upon combining thiol-terminated tetra-arm polyethylene glycol (PEG) polymers with linear telechelic PEG-based polymers containing pyridyl disulfide units at their chain ends. Rapid gelation proceeds with good conversions (>85%) to yield macroporous hydrogels possessing high water uptake. Furthermore, due to the presence of the disulfide linkages, the thus-obtained hydrogels can self-heal. The obtained hydrogels undergo complete degradation when exposed to environments rich in thiol-containing agents such as dithiothreitol (DTT) and L-glutathione (GSH). Also, the release profile of encapsulated protein, namely, bovine serum albumin, can be tuned by varying the molecular weight of the polymeric precursors. Additionally, it was demonstrated that complete dissolution of the hydrogel to rapidly release the encapsulated protein occurs upon treating these hydrogels with DTT. Cytotoxicity evaluation of the hydrogels and their degradation products indicated the benign nature of these hydrogels. Additionally, the cytocompatible nature of these materials was also evident from a live/dead cell viability assay. One can envision that the facile fabrication and their ability to degrade on-demand and release their payload will make these benign polymeric scaffolds attractive for various biomedical applications.}},
  author       = {{Kilic Boz, Ruveyda and Aydin, Duygu and Kocak, Salli and Golba, Bianka and Sanyal, Rana and Sanyal, Amitav}},
  issn         = {{1043-1802}},
  journal      = {{BIOCONJUGATE CHEMISTRY}},
  keywords     = {{Organic Chemistry,Pharmaceutical Science,Pharmacology,Biomedical Engineering,Bioengineering,Biotechnology,POLY(ETHYLENE GLYCOL) HYDROGELS,DELIVERY,COPOLYMERS,FUNCTIONALIZATION,DISSOLUTION,FABRICATION,NANOGELS}},
  language     = {{eng}},
  number       = {{5}},
  pages        = {{839--847}},
  title        = {{Redox-responsive hydrogels for tunable and 'on-demand' release of biomacromolecules}},
  url          = {{http://doi.org/10.1021/acs.bioconjchem.2c00094}},
  volume       = {{33}},
  year         = {{2022}},
}

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