Rigidity-dependent formation process of DNA supramolecular hydrogels
Source abstract
Abstract
Abstract A DNA building block with tunable rigidity was constructed, and the corresponding hydrogel formation process was investigated accordingly. A high rigidity was demonstrated to facilitate fast gelation. Different gelation pathways of the rigid and flexible building blocks were revealed, and a cyclized dimer intermediate was proposed. The energy barrier of the ring-opening process was also shown to play a fundamental role in determining the gelation kinetics. Furthermore, the hydrogel molecular network rigidity was also tuned in situ through strand displacement, which also supports the kinetic control mechanism of the formation process of DNA hydrogels.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Advanced biosensing and bioanalysis techniques · RNA Interference and Gene Delivery · DNA and Nucleic Acid Chemistry
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (44)
Show source-provided references
1. Appel, E. A., del Barrio, J., Loh, X. J. & Scherman, O. A. Supramolecular polymeric hydrogels. Chem. Soc. Rev. 41, 6195–6214 (2012).10.1039/c2cs35264h ↗
2. Yang, C. H. & Suo, Z. G. Hydrogel ionotronics. Nat. Rev. Mater. 3, 125–142 (2018).10.1038/s41578-018-0018-7 ↗
3. Ahmed, E. M. Hydrogel: preparation, characterization, and applications: a review. J. Adv. Res. 6, 105–121 (2015).10.1016/j.jare.2013.07.006 ↗
4. Li, J. et al. Short and simple peptide-based pH-sensitive hydrogel for antitumor drug delivery. Chin. Chem. Lett. 33, 1936–1940 (2022).10.1016/j.cclet.2021.10.058 ↗
5. Plamper, F. A. & Richtering, W. Functional microgels and microgel systems. Acc. Chem. Res. 50, 131–140 (2017).10.1021/acs.accounts.6b00544 ↗
6. Lutolf, M. P. Spotlight on hydrogels. Nat. Mater. 8, 451–453 (2009).10.1038/nmat2458 ↗
7. Liu, X. Y., Liu, J., Lin, S. T. & Zhao, X. H. Hydrogel machines. Mater. Today 36, 102–124 (2020).10.1016/j.mattod.2019.12.026 ↗
8. Nagahara, S. & Matsuda, T. Hydrogel formation via hybridization of oligonucleotides derivatized in water-soluble vinyl polymers. Polym. Gels Netw. 4, 111–127 (1996).10.1016/0966-7822(96)00001-9 ↗
9. Li, F., Tang, J. P., Geng, J. H., Luo, D. & Yang, D. Y. Polymeric DNA hydrogel: design, synthesis and applications. Prog. Polym. Sci. 98, 101163 (2019).10.1016/j.progpolymsci.2019.101163 ↗
10. Li, F. Y., Lyu, D. Y., Liu, S. & Guo, W. W. DNA hydrogels and microgels for biosensing and biomedical applications. Adv. Mater. 32, 1806538 (2020).10.1002/adma.201806538 ↗
11. Shi, J. Z., Shi, Z. W., Dong, Y. C., Wu, F. & Liu, D. S. Responsive DNA-based supramolecular hydrogels. ACS Appl. Bio Mater. 3, 2827–2837 (2020).10.1021/acsabm.0c00081 ↗
12. Dong, Y. H. et al. DNA functional materials assembled from branched DNA: design, synthesis, and applications. Chem. Rev. 120, 9420–9481 (2017).10.1021/acs.chemrev.0c00294 ↗
13. Shao, Y., Jia, H. Y., Cao, T. Y. & Liu, D. S. Supramolecular hydrogels based on DNA self-assembly. Acc. Chem. Res. 50, 659–668 (2017).10.1021/acs.accounts.6b00524 ↗
14. Jin, J. et al. A triggered DNA hydrogel cover to envelop and release single cells. Adv. Mater. 25, 4714–4717 (2013).10.1002/adma.201301175 ↗
15. Yang, B. et al. Shear-thinning and designable responsive supramolecular DNA hydrogels based on chemically branched DNA. ACS Appl. Mater. Interfaces 13, 48414–48422 (2021).10.1021/acsami.1c15494 ↗
16. Li, C. et al. Rapid formation of a supramolecular polypeptide-DNA hydrogel for in situ three-dimensional multilayer bioprinting. Angew. Chem. Int. Ed. 54, 3957–3961 (2015).10.1002/anie.201411383 ↗
17. Li, C. et al. A writable polypeptide–DNA hydrogel with rationally designed multi-modification sites. Small 11, 1138–1143 (2015).10.1002/smll.201401906 ↗
18. Peng, L. et al. Macroscopic volume change of dynamic hydrogels induced by reversible DNA hybridization. J. Am. Chem. Soc. 134, 12302–12307 (2012).10.1021/ja305109n ↗
19. Chen, E. J. et al. A pH-triggered, fast-responding DNA hydrogel. Angew. Chem. Int. Ed. 48, 7660–7663 (2009).10.1002/anie.200902538 ↗
20. Liu, H. Y., Cao, T. Y., Xu, Y., Dong, Y. C. & Liu, D. S. Tuning the mechanical properties of a DNA hydrogel in three phases based on ATP aptamer. Int. J. Mol. Sci. 19, 1633 (2018).10.3390/ijms19061633 ↗
21. Li, C. et al. Responsive double network hydrogels of interpenetrating DNA and CB[8] host-guest supramolecular systems. Adv. Mater. 27, 3298–3304 (2015).10.1002/adma.201501102 ↗
22. Vázquez-González, M. & Willner, I. Stimuli-responsive biomolecule-based hydrogels and their applications. Angew. Chem. Int. Ed. 59, 15342–15377 (2020).10.1002/anie.201907670 ↗
23. Lu, C. H., Guo, W. W., Hu, Y. W., Qi, X. J. & Willner, I. Multitriggered shape-memory acrylamide–DNA hydrogels. J. Am. Chem. Soc. 137, 15723–15731 (2015).10.1021/jacs.5b06510 ↗
24. Ren, J. T. et al. pH-responsive and switchable triplex-based DNA hydrogels. Chem. Sci. 6, 4190–4195 (2015).10.1039/C5SC00594A ↗
25. Yang, B. et al. A biostable L-DNA hydrogel with improved stability for biomedical applications. Angew. Chem. Int. Ed. 61, e202202520 (2022).10.1002/anie.202202520 ↗
26. Wu, J. Y. et al. Self-assembly of dendritic DNA into a hydrogel: application in three-dimensional cell culture. ACS Appl. Mater. Interfaces 13, 49705–49712 (2021).10.1021/acsami.1c14445 ↗
27. Yuan, T. Y. et al. Highly permeable DNA supramolecular hydrogel promotes neurogenesis and functional recovery after completely transected spinal cord injury. Adv. Mater. 33, 2102428 (2021).10.1002/adma.202102428 ↗
28. Yan, X. et al. Anti-friction MSCs delivery system improves the therapy for severe osteoarthritis. Adv. Mater. 33, 2104758 (2021).10.1002/adma.202104758 ↗
29. Joseph, K. A., Dave, N. & Liu, J. W. Electrostatically directed visual fluorescence response of DNA-functionalized monolithic hydrogels for highly sensitive Hg2+ detection. ACS Appl. Mater. Interfaces 3, 733–739 (2011).10.1021/am101068c ↗
30. Huang, Y. S. et al. Target-responsive DNAzyme cross-linked hydrogel for visual quantitative detection of lead. Anal. Chem. 86, 11434–11439 (2014).10.1021/ac503540q ↗
31. Li, J. et al. Self-assembly of DNA nanohydrogels with controllable size and stimuli-responsive property for targeted gene regulation therapy. J. Am. Chem. Soc. 137, 1412–1415 (2015).10.1021/ja512293f ↗
32. Ding, F. et al. A crosslinked nucleic acid nanogel for effective siRNA delivery and antitumor therapy. Angew. Chem. Int. Ed. 57, 3064–3068 (2018).10.1002/anie.201711242 ↗
33. Mo, F. L. et al. DNA hydrogel-based gene editing and drug delivery systems. Adv. Drug Deliv. Rev. 168, 79–98 (2021).10.1016/j.addr.2020.07.018 ↗
34. Zhou, X. et al. Reversibly tuning the mechanical properties of a DNA hydrogel by a DNA nanomotor. Chem. Commun. 52, 10668–10671 (2016).10.1039/C6CC04724F ↗
35. Wu, F. et al. Self-collapsing of single molecular poly-propylene oxide (PPO) in a 3D DNA network. Small 14, 1703462 (2018).
36. Xing, Z. Y. et al. Microrheology of DNA hydrogels. Proc. Natl Acad. Sci. USA 115, 8137–8142 (2018).10.1073/pnas.1722206115 ↗
37. Stoev, I. D. et al. On the role of flexibility in linker-mediated DNA hydrogels. Soft. Mater. 16, 990–1001 (2020).10.1039/C9SM01398A ↗
38. Huang, Z. H. et al. Supramolecular polymerization promoted and controlled through self-sorting. Angew. Chem. Int. Ed. 53, 5351–5355 (2014).10.1002/anie.201402817 ↗
39. Jia, H. Y. et al. Controllable supramolecular “ring opening” polymerization based on DNA duplex. Polymer 171, 121–126 (2019).10.1016/j.polymer.2019.03.025 ↗
40. Zhang, W. et al. Controllable fabrication of a supramolecular polymer incorporating twisted cucurbit[14]uril and cucurbit[8]uril via self-sorting. Chin. Chem. Lett. 33, 2455–2458 (2022).10.1016/j.cclet.2021.11.053 ↗
41. Yang, D. Y. et al. DNA materials: bridging nanotechnology and biotechnology. Acc. Chem. Res. 47, 1902–1911 (2014).10.1021/ar5001082 ↗
42. Smith, S. B., Cui, Y. J. & Bustamante, C. Overstretching B-DNA: the elastic. response of individual double-stranded and single-stranded DNA molecules. Science 271, 795–799 (1996).10.1126/science.271.5250.795 ↗
43. Baumann, C. G., Smith, S. B., Bloomfield, V. A. & Bustamante, C. Ionic effects on the elasticity of single DNA molecules. Proc. Natl Acad. Sci. USA 94, 6185–6190 (1997).10.1073/pnas.94.12.6185 ↗
44. Mitchell, J. S., Glowacki, J., Grandchamp, A. E., Manning, R. S. & Maddocks, J. H. Sequence-dependent persistence lengths of DNA. J. Chem. Theory Comput. 13, 1539–1555 (2017).10.1021/acs.jctc.6b00904 ↗