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Decahexanuclear Zinc(II) Coordination Container Featuring a Flexible Tetracarboxylate Ligand: A Self-Assembly Supermolecule for Highly Efficient Drug Delivery of Anti-Inflammatory Agents

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posted on 16.07.2021, 19:38 by Can He, Xuzhuo Chen, Cheng-Zhe Sun, Li-Yi Zhang, Weifeng Xu, Shanyong Zhang, Zhenqiang Wang, Feng-Rong Dai
The application of a coordination container in biomedicine is hindered by single binding domains and unsatisfactory biostability and biocompatibility. Herein, we designed a sulfonylcalix[4]­arene-based decahexanuclear zinc­(II) coordination container employing a flexible tetracarboxylate ligand as a linker and utilized it as a novel drug delivery system. The coordination container consisting of one endo and four exo cavities provides multiple binding domains for efficient encapsulation of drug molecules as clearly revealed by systematic host–guest studies using NMR techniques of 1H NMR titration experiments and 2D NOESY and diffusion-ordered NMR spectroscopy studies. Incorporation of a flexible p-phenylene-bis­(methanamino) spacer into the container via the carboxylate linker allowed a stepwise drug loading process through sequential binding at endo and exo cavities, as well as enabling pH-responsive stepwise drug release. The drug-loaded coordination container not only exhibits excellent biostability and biocompatibility but also provides encouraging therapeutic efficiency toward inflammatory macrophages as revealed by in vitro studies. The novel strategy for engineering the endo cavity of a coordination container provides a new approach to achieving controlled drug delivery and opens up new opportunities for designing novel functional supramolecular materials.

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