Zhong Qi-Zhi, Richardson Joseph J, Tian Yuan, Tian Haijiang, Cui Jiwei, Mann Stephen, Caruso Frank
Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria, 3010, Australia.
Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education, School of Chemistry and Chemical Engineering, Shandong University, Jinan, Shandong, 250100, P. R. China.
Angew Chem Int Ed Engl. 2023 Mar 27;62(14):e202218021. doi: 10.1002/anie.202218021. Epub 2023 Feb 20.
Nanostructured materials with tunable structures and functionality are of interest in diverse areas. Herein, metal ions are coordinated with quinones through metal-acetylacetone coordination bonds to generate a class of structurally tunable, universally adhesive, hydrophilic, and pH-degradable materials. A library of metal-quinone networks (MQNs) is produced from five model quinone ligands paired with nine metal ions, leading to the assembly of particles, tubes, capsules, and films. Importantly, MQNs show bidirectional pH-responsive disassembly in acidic and alkaline solutions, where the quinone ligands mediate the disassembly kinetics, enabling temporal and spatial control over the release of multiple components using multilayered MQNs. Leveraging this tunable release and the inherent medicinal properties of quinones, MQN prodrugs with a high drug loading (>89 wt %) are engineered using doxorubicin for anti-cancer therapy and shikonin for the inhibition of the main protease in the SARS-CoV-2 virus.
具有可调节结构和功能的纳米结构材料在多个领域都备受关注。在此，金属离子通过金属 - 乙酰丙酮配位键与醌类配位，生成一类结构可调节、具有普遍粘附性、亲水性且可在特定pH值下降解的材料。由五种模型醌配体与九种金属离子形成了一个金属 - 醌网络（MQN）库，从而组装出颗粒、管状、胶囊状和薄膜状结构。重要的是，MQN在酸性和碱性溶液中表现出双向pH响应性解离，其中醌配体介导了解离动力学，使得利用多层MQN能够对多种成分的释放进行时空控制。利用这种可调节释放以及醌类固有的药用特性，使用阿霉素进行抗癌治疗以及使用紫草素抑制SARS-CoV-2病毒的主要蛋白酶，设计出了具有高药物负载量（>89 wt %）的MQN前药。
