Freiburg Materials Research Center, University of Freiburg, Stefan-Meier-Straße 21, 79104 Freiburg, Germany.
Freiburg Center for Interactive Materials and Bioinspired Technologies, University of Freiburg, Georges-Köhler-Allee 105, 79110 Freiburg, Germany.
ACS Macro Lett. 2021 Jun 15;10(6):671-678. doi: 10.1021/acsmacrolett.1c00211. Epub 2021 May 13.
DNA mechanosensors offer unique properties for mechano-adaptive and self-reporting materials, such as programmable bond strength and geometrical strain response, tunable fluorescent strain sensing, interfacing to biological systems, and the ability to store mechanical information. However, the facile incorporation of advanced DNA motifs into polymer networks and achieving robustness in application settings remain difficult. Herein, we introduce one-component DNA mechanoprobes that can be easily polymerized into polymer hydrogels and even elastomers to allow strain-induced fluorescence sensing. The all-in-one mechanoprobe contains a DNA hairpin for programmable force sensing, an internal fluorophore-quencher pair as a reporter, and methacrylamide groups on both ends for rapid and facile photopolymerization into networks based on the nontoxic water-soluble monomer methoxy triethylene glycol acrylate (mTEGA). In addition to mechanosensing hydrogels, we utilize the low of p(mTEGA) to develop the first bulk elastomer materials with DNA force sensors, which show high elasticity and stronger mechanofluorescence. The system makes decisive steps forward for DNA-based mechanoprobes by overcoming the classical multicomponent design of such probes, allowing photopolymerization useful for the design of complex objects or even 3D printing and demonstrating that such motifs may even be useful in dry bulk materials.
DNA 机械感受器为机械自适应和自报告材料提供了独特的特性,例如可编程键强度和几何应变响应、可调谐荧光应变传感、与生物系统的接口以及存储机械信息的能力。然而,将先进的 DNA 基序轻松纳入聚合物网络并在应用环境中实现稳健性仍然具有挑战性。在此,我们引入了一种单一组分的 DNA 机械探针,可轻松聚合到聚合物水凝胶中,甚至弹性体中,以实现应变诱导的荧光传感。这种一体化机械探针包含一个用于可编程力感应的 DNA 发夹、一个内部荧光团猝灭剂对作为报告器,以及两端的甲基丙烯酰胺基团,用于基于低毒水溶性单体甲氧基三乙二醇丙烯酸酯 (mTEGA) 的快速简便的光聚合形成网络。除了机械传感水凝胶之外,我们还利用低 p(mTEGA) 值来开发具有 DNA 力传感器的第一批块状弹性体材料,这些材料表现出高弹性和更强的机械荧光。该系统通过克服此类探针的经典多组分设计向前迈出了决定性的一步,允许光聚合用于设计复杂物体,甚至 3D 打印,并证明这些基序甚至可能在干燥的块状材料中有用。