Key Laboratory of Biomedical Polymers-Ministry of Education, College of Chemistry and Molecular Sciences, and ‡UC Berkeley-Wuhan University Joint Innovative Center, The Institute of Advanced Studies, Wuhan University , Luojiashan, Wuhan 430072, China.
J Am Chem Soc. 2017 Oct 11;139(40):14209-14216. doi: 10.1021/jacs.7b07392. Epub 2017 Sep 28.
We report the control of guest release profiles by dialing-in desirable interactions between guest molecules and pores in metal-organic frameworks (MOFs). The interactions can be derived by the rate constants that were quantitatively correlated with the type of functional group and its proportion in the porous structure; thus the release of guest molecules can be predicted and programmed. Specifically, three probe molecules (ibuprofen, rhodamine B, and doxorubicin) were studied in a series of robust and mesoporous MOFs with multiple functional groups [MIL-101(Fe)-(NH), MIL-101(Fe)-(CH), and MIL-101(Fe)-(CH)(NH)]. The release rate can be adjusted by 32-fold [rhodamine from MIL-101(Fe)-(NH)], and the time of release peak can be shifted by up to 12 days over a 40-day release period [doxorubicin from MIL-101(Fe)-(CH)(NH)], which was not obtained in the physical mixture of the single component MOF counterparts nor in other porous materials. The corelease of two pro-drug molecules (ibuprofen and doxorubicin) was also achieved.
我们通过调节客体分子与金属-有机骨架(MOFs)孔道之间的期望相互作用来控制客体释放特性。这种相互作用可以通过速率常数来定量关联,而速率常数又与官能团的类型及其在多孔结构中的比例有关;因此,可以预测和设计客体分子的释放。具体来说,我们在一系列具有多种官能团的坚固介孔 MOFs 中研究了三种探针分子(布洛芬、罗丹明 B 和阿霉素)[MIL-101(Fe)-(NH)、MIL-101(Fe)-(CH)和 MIL-101(Fe)-(CH)(NH)]。释放速率可以调节 32 倍[MIL-101(Fe)-(NH)中的罗丹明 B],在 40 天的释放期内,释放峰时间可以最多延迟 12 天[MIL-101(Fe)-(CH)(NH)中的阿霉素],而在单一成分 MOF 对应物的物理混合物或其他多孔材料中并未获得这种效果。两种前药分子(布洛芬和阿霉素)的共释放也得以实现。