Multitriggered Shape-Memory Acrylamide-DNA Hydrogels
Multitriggered Shape-Memory Acrylamide-DNA Hydrogels
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DOI：
10.1021/jacs.5b06510
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发表时间：
2015-12-23
影响因子：
15
通讯作者：
Willner, Itamar
中科院分区：
文献类型：
--
作者：
Lu, Chun-Hua;Guo, Weiwei;Willner, Itamar
丙烯酰胺-丙烯酰胺核酸通过两个协同的功能基序交联以形成成形的丙烯酰胺-DNA水凝胶。其中一个交联动机响应于外部触发，导致其中一个刺激响应桥的解离，并且导致刚性形状的水凝胶转变成软的无形状状态，其中由于链缠结，残留的桥接单元为水凝胶的重塑提供了内在记忆。使无形状的状态经受反刺激以恢复解离的桥，并再生水凝胶的原始形状。通过刺激响应桥的循环解离和重新组装，证明了水凝胶在刚性形状的水凝胶结构和柔软的无形状状态之间的可逆可切换转变。描述了通过K+稳定的G-四链体/双链体单元、通过i-基序/双链体单元或通过两个不同的双链体桥桥接的成形水凝胶。在适当的触发剂和反触发剂（K+离子/冠醚; pH = 5.0/8.0;燃料/反燃料链）的存在下，刺激水凝胶在成形和非成形状态之间的循环转变。将形状记忆水凝胶整合到成形的两水凝胶或三水凝胶混合结构中。证明了在成形水凝胶和无定形状态之间的混合结构的选择性结构域的循环程序化转变。讨论了形状记忆水凝胶在传感、信息记录和负载控制释放方面的可能应用。
Acrylamide acrylamide nucleic acids are cross-linked by two cooperative functional motives to form shaped acrylamide-DNA hydrogels. One of the cross-linking motives responds to an external trigger, leading to the dissociation of one of the stimuli-responsive bridges, and to the transition of the stiff shaped hydrogels into soft shapeless states, where the residual bridging units, due to the chains entanglement, provide an intrinsic memory for the reshaping of the hydrogels. Subjecting the shapeless states to counter stimuli restores the dissociated bridges, and regenerates the original shape of the hydrogels. By the cyclic dissociation and reassembly of the stimuli-responsive bridges, the reversible switchable transitions of the hydrogels between stiff shaped hydrogel structures and soft shapeless states are demonstrated. Shaped hydrogels bridged by K+-stabilized G-quadruplexes/duplex units, by i-motif/duplex units, or by two different duplex bridges are described. The cyclic transitions of the hydrogels between shaped and shapeless states are stimulated, in the presence of appropriate triggers and counter triggers (K+ ion/crown ether; pH = 5.0/8.0; fuel/antifuel strands). The shape-memory hydrogels are integrated into shaped two-hydrogel or three-hydrogel hybrid structures. The cyclic programmed transitions of selective domains of the hybrid structures between shaped hydrogel and shapeless states are demonstrated. The possible applications of the shape-memory hydrogels for sensing, inscription of information, and controlled release of loads are discussed.