Solvent-Assisted Self-Assembly of a Metal-Organic Framework Based Biocatalyst for Cascade Reaction Driven Photodynamic Therapy

Solvent-Assisted Self-Assembly of a Metal-Organic Framework Based Biocatalyst for Cascade Reaction Driven Photodynamic Therapy
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DOI:
10.1021/jacs.0c02497
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发表时间:
2020-04-08
影响因子:
15
通讯作者:
Chen, Xiaoyuan
Chen, Xiaoyuan
中科院分区:
化学1区
文献类型:
--
作者:
He, Liangcan;Ni, Qianqian;Chen, Xiaoyuan

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活细胞中的生物催化反应涉及空间受限的微环境中的复杂转变。受生物转化过程的启发,我们通过将人工酶(超小Au纳米颗粒)与上转换纳米颗粒(NaYF4@NaYb0.92F4:Er-0.08@NaYF4)锆/铁卟啉金属有机框架核壳纳米颗粒(UMOF NPs)整合,在荷瘤小鼠中展示了有效的生物催化级联驱动的光动力学疗法,所述纳米颗粒充当生物催化剂和纳米反应器。核壳结构的UMOF纳米粒子的构建是通过一种独特的“溶剂辅助自组装”方法实现的。超小AuNP在UMOFs基质上的整合导致葡萄糖耗尽,通过葡萄糖氧化酶样催化活性提供Au介导的癌症治疗。同时,UMOF基质通过在照射时经由过氧化氢分解连续供应氧而充当近红外(NIR)光光子激活的单线态氧发生器。这类生物催化剂为生物医学、催化和能源应用提供了令人兴奋的机会。
Biocatalytic reactions in living cells involve complex transformations in the spatially confined microenvironments. Inspired by biological transformation processes, we demonstrate effective biocatalytic cascade driven photodynamic therapy in tumor-bearing mice by the integration of an artificial enzyme (ultrasmall Au nanoparticles) with upconversion nanoparticles (NaYF4@NaYb0.92F4:Er-0.08@NaYF4)zirconium/iron porphyrin metal-organic framework core-shell nanoparticles (UMOF NPs) which act as biocatalysts and nanoreactors. The construction of core-shell UMOF NPs are realized by using a unique "solvent-assisted self-assembly" method. The integration of ultrasmall AuNPs on the UMOFs matrix leads to glucose depletion, providing Au-mediated cancer therapy via glucose oxidase like catalytic activity. Meanwhile, the UMOF matrix acts as a near-infrared (NIR) light photon-activated singlet oxygen generator through a continuous supply of oxygen via hydrogen peroxide decomposition upon irradiation. Such kinds of biocatalysts offer exciting opportunities for biomedical, catalytical,and energy applications.