Fluorescent Metallacage-Core Supramolecular Polymer Gel Formed by Orthogonal Metal Coordination and Host-Guest Interactions.
Fluorescent Metallacage-Core Supramolecular Polymer Gel Formed by Orthogonal Metal Coordination and Host-Guest Interactions.
复制标题
正交金属配位和主客体相互作用形成的荧光金属笼核超分子聚合物凝胶
DOI：
10.1021/jacs.8b03781
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发表时间：
2018-06-20
影响因子：
15
通讯作者：
Stang PJ
中科院分区：
文献类型：
--
作者：
Lu C;Zhang M;Tang D;Yan X;Zhang Z;Zhou Z;Song B;Wang H;Li X;Yin S;Sepehrpour H;Stang PJ
本文报道了利用正交金属配位和主客体相互作用制备多功能金属配合物核超分子凝胶。首次通过金属配位驱动的顺式Pt（PEt 3）2（OTf）2、四苯乙烯（TPE）基苯甲酸钠配体和线性联吡啶配体的自组装反应，制备了一种在柱部分附加四个21-冠-7（21 C7）基团的四元棱柱笼.进一步向笼中加入双铵连接体，通过21 C7部分和铵盐之间的主客体相互作用产生超分子聚合物网络，其在相对较高的浓度下形成超分子凝胶。由于掺入TPE衍生物作为荧光团，凝胶显示出发射特性。由于动态的金属配位作用和主客体相互作用稳定了整个网络结构，还观察到了多重刺激响应性和良好的自修复特性。此外，凝胶的储能模量和损耗模量是没有金属层芯的凝胶的10倍，表明刚性金属层在增强凝胶的刚度方面起着重要作用。本文所述的研究不仅丰富了荧光金属配合物的功能化通过优雅的配体设计，而且还提供了一种方法来制备刺激响应和自我修复的超分子凝胶作为稳健和智能材料。
Herein, we report the preparation of a multi-functional metallacage-cored supramolecular gel by orthogonal metal-coordination and host-guest interactions. A tetragonal prismatic cage with four appended 21-crown-7 (21C7) moieties in its pillar parts was first prepared via the metal-coordination-driven self-assembly of cis-Pt(PEt3)2(OTf)2, tetraphenylethene (TPE) based sodium benzoate ligands and linear dipyridyl ligands. Further addition of a bisammonium linker to the cage delivered a supramolecular polymer network via the host-guest interactions between the 21C7 moieties and ammonium salts, which formed a supramolecular gel at relatively higher concentrations. Due to the incorporation of a TPE derivative as the fluorophore, the gel shows emission properties. Multiple stimuli-responsiveness and good self-healing properties were also observed because of the dynamic metal-coordination and host-guest interactions used to stabilize the whole network structure. Moreover, the storage and loss moduli of the gel are 10-fold of the gel without the metallacage cores, indicating that the rigid metallacage plays a significant role in enhancing the stiffness of the gel. The studies described herein not only enrich the functionalization of fluorescent metallacages via elegant ligand design but also provide a way to prepare stimuli-responsive and self-healing supramolecular gels as robust and smart materials.
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