Lee, S. R., Ong, C. Y. J., Wong, J. Y., Ke, Y., Lim, J. Y. C., Dong, Z., Long, Y., & Hu, Y. (2024). Programming the Assembly of Oligo-Adenine with Coralyne into a pH-Responsive DNA Hydrogel. ACS Applied Materials & Interfaces, 16(12), 15394–15404. https://
doi.org/10.1021/acsami.4c01678
Abstract:
External stimuli-responsive DNA hydrogels present interesting platforms for drug loading and triggered release. Typically, drug molecules are encapsulated within three-dimensionally hybridized DNA networks. However, the utilization of drug molecules as cofactors to facilitate the directed assembly of DNA strands into hydrogel frameworks and their subsequent controlled release remains to be explored. Herein, we introduce the guided assembly of oligo-adenine (A-strand) into an acidic pH-responsive DNA hydrogel using an anticancer drug, coralyne (COR), as a low-molecular-weight cofactor. At pH 7, COR orchestrates the assembly of A-strand into an antiparallel duplex configuration cross-linked by A-COR-A units at a stoichiometric ratio of one COR cofactor per four adenine bases, resulting in a DNA hydrogel characterized by A-COR-A duplex bridges. At pH 4–5, the instability of A-COR-A units results in the disintegration of the duplex into its constituent components, leading to the release of COR and simultaneous dissociation of the DNA hydrogel matrix. This study introduces a method by which drug molecules, exemplified here by COR, facilitate the direct formation of a supramolecular cofactor-DNA complex, subsequently leading to the creation of a stimuli-responsive DNA hydrogel. This approach may inspire future investigations into DNA hydrogels tailored for controlled drug encapsulation and release applications.
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Funding Info:
This research / project is supported by the A*STAR - Career Development Fund
Grant Reference no. : C210112014
This research is supported by core funding from: SERC
Grant Reference no. : NA
This research / project is supported by the A*STAR - Central Research Fund
Grant Reference no. : KIMR220901aSERCRF
This research / project is supported by the A*STAR - IAF-PP
Grant Reference no. : H20c6a0033
This research / project is supported by the A*STAR / National Research Foundation - Quantum Engineering Programme 2.0
Grant Reference no. : NRF2021-QEP2-03-P09