open access

https://hdl.handle.net/2115/88857

Star-Polymer-DNA Gels Showing Highly Predictable and Tunable Mechanical Responses

英語

viscoelasticity

2022-04-01

Wiley-Blackwell

Advanced Materials

34(13)

2108818

Dynamically crosslinked gels are appealing materials for applications that require time-dependent mechanical responses. DNA duplexes are ideal crosslinkers for building such gels because of their excellent sequence addressability and flexible tunability in bond energy. However, the mechanical responses of most DNA gels are complicated and unpredictable. Here, a DNA gel with a highly homogeneous gel network and well predictable mechanical behaviors is demonstrated by using a pair of star-polymer-DNA precursors with presimulated DNA sequences showing the two-state transition. The melting curve analysis of the DNA gels reveals the good correspondence between the thermodynamic potentials of the DNA crosslinkers and the presimulated values by DNA calculators. Stress-relaxation tests and dissociation kinetics measurements show that the macroscopic relaxation time of the DNA gels is approximately equal to the lifetime of the DNA crosslinkers over 4 orders of magnitude from 0.1-2000 s. Furthermore, a series of durability tests find the DNA gels are hysteresis-less and self-healable after the applications of repeated temperature and mechanical stimuli. These results demonstrate the great potential of star-polymer-DNA precursors for building gels with predictable and tunable viscoelastic properties, suitable for applications such as stress-response extracellular matrices, injectable solids, and soft robotics.

学術雑誌論文

Accepted Manuscript

This is the peer reviewed version of the following article: Ohira, M., Katashima, T., Naito, M., Aoki, D., Yoshikawa, Y., Iwase, H., Takata, S.-i., Miyata, K., Chung, U.-i., Sakai, T., Shibayama, M., Li, X., Star-Polymer–DNA Gels Showing Highly Predictable and Tunable Mechanical Responses. Adv. Mater. 2022, 34, 2108818, which has been published in final form at https://doi.org/10.1002/adma.202108818. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.

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