文献类型：期刊文献

英文题名：Multi-triggered Supramolecular DNA/Bipyridinium Dithienylethene Hydrogels Driven by Light, Redox, and Chemical Stimuli for Shape-Memory and Self-Healing Applications

作者：Li, Ziyuan[1,2];Davidson-Rozenfeld, Gilad[3];Vazquez-Gonzalez, Margarita[3];Fadeev, Michael[3];Zhang, Junji[1,2];Tian, He[1,2];Willner, Itamar[3]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Joint Int Res Lab Precis Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Hebrew Univ Jerusalem, Inst Chem, Minerva Ctr Biohybrid Complex Syst, IL-91904 Jerusalem, Israel

年份：2018

卷号：140

期号：50

起止页码：17691

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20185106268160);WOS:【SCI-EXPANDED(收录号:WOS:000454383400051)】；

基金：The authors acknowledge financial support from the NSFC (21420102004, 21878086), the Israel Science Foundation, Shanghai Municipal Science and Technology Major Project (2018SHZDZX03), and the international cooperation program of Shanghai Science and Technology Committee (17520750100).

语种：英文

外文关键词：Crown ethers - Nucleic acids - Amines - Neurophysiology - Ethers - Scaffolds - Self-healing materials - Supramolecular chemistry - Crosslinking - Hydrogels

摘要：Multi-triggered DNA/bipyridinium dithienylethene (DTE) hybrid carboxymethyl cellulose (CMC)-based hydrogels are introduced. DTE exhibits cyclic and reversible photoisomerization properties, switching between the closed state (DTEc), the electron acceptor, and the open isomer (DTEo) that lacks electron acceptor properties. One system introduces a dual stimuli-responsive hydrogel containing CMC chains modified with electron donor dopamine sites and self-complementary nucleic acids. In the presence of DTEC and the CMC scaffold, a stiff hydrogel is formed, cooperatively stabilized by dopamine/DTEc donor-acceptor interactions and by duplex nucleic acids. The cyclic and reversible formation and dissociation of the supramolecular donor-acceptor interactions, through light-induced photoisomerization of DTE, or via oxidation and subsequent reduction of the dopamine sites, leads to hydrogels of switchable stiffness. Another system introduces a stimuli-responsive hydrogel triggered by one of three alternative signals. The stiff, multi-triggered hydrogel consists of CMC chains cross-linked by dopamine/DTEc donor-acceptor interactions, and by supramolecular K+-stabilized G-quadruplexes. The G-quadruplexes are reversibly separated in the presence of 18-crown-6 ether and reformed upon the addition of Kt The stiff hydrogel undergoes reversible transitions between high-stiffness and low-stiffness states triggered by light, redox agents, or K+/crown ether. The hybrid donor-acceptor/G-quadruplex cross-linked hydrogel shows shape-memory and self-healing features. By using three different triggers and two alternative memory-codes, e.g., the dopamine/DTEc or the K+-stabilized G-quadruplexes, the guided shape-memory function of the hydrogel matrices is demonstrated.