Stiffness-switchable DNA-based constitutional dynamic network hydrogels for self-healing and matrix-guided controlled chemical processes

Liang Yue, Shan Wang, Verena Wulf and Itamar Willner ()
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Liang Yue: The Hebrew University of Jerusalem
Shan Wang: The Hebrew University of Jerusalem
Verena Wulf: The Hebrew University of Jerusalem
Itamar Willner: The Hebrew University of Jerusalem

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Constitutional dynamic networks (CDNs) attract interest as signal-triggered reconfigurable systems mimicking natural networks. The application of CDNs to control material properties is, however, a major challenge. Here we report on the design of a CDN consisting of four toehold-modified constituents, two of which act as bidentate units for chain-elongating, while the other two form a tetradentate structure acting as a crosslinking unit. Their hybridization yields a hydrogel of medium stiffness controlled by the balance between bidentate and tetradentate units. Stabilization of the tetradentate constituent by an auxiliary effector up-regulates the crosslinking unit, yielding a high-stiffness hydrogel. Conversely, stabilization of one of the bidentate constituents by an orthogonal effector enriches the chain-elongation units leading to a low-stiffness hydrogel. Using appropriate counter effectors, the hydrogels are reversibly switched across low-, medium- and high-stiffness states. The hydrogels are used to develop self-healing and controlled drug-release matrices and functional materials for operating biocatalytic cascades.

Date: 2019
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DOI: 10.1038/s41467-019-12697-2

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