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过渡金属 Ru(II)催化剂固定化纳米反应器用于细胞条件生物正交催化。

Transition Metal Ru(II) Catalysts Immobilized Nanoreactors for Conditional Bioorthogonal Catalysis in Cells.

机构信息

State Key Laboratory of Natural Medicines, Jiangsu Key Laboratory of Drug Discovery for Metabolic Diseases, Center of Advanced Pharmaceuticals and Biomaterials, China Pharmaceutical University, Nanjing 210009, China.

School of Life Sciences and Technology, Xinxiang Medical University, Xinxiang 453003, China.

出版信息

ACS Appl Mater Interfaces. 2024 Apr 3;16(13):15870-15878. doi: 10.1021/acsami.3c19133. Epub 2024 Mar 23.

DOI:10.1021/acsami.3c19133
PMID:38520329
Abstract

Employing transition metal catalysts (TMCs) to perform bioorthogonal activation of prodrugs and pro-fluorophores in biological systems, particularly in a conditional fashion, remains a challenge. Here, we used a mesoporous organosilica nanoscaffold (RuMSN), which localizes Ru(II) conjugates on the pore wall, enabling the biorthogonal photoreduction reactions of azide groups. Due to easily adjustable surface charges and pore diameter, this efficiently engineering RuMSN catalyst, with abundant active sites on the inner pore well, could spontaneously repel or attract substrates with different molecular sizes and charges and thus ensure selective bioorthogonal catalysis. Depending on it, engineering RuMSN nanoreactors showed fascinating application scales from conditional bioorthogonal activation of prodrugs and pro-fluorophores in either intra- or extracellular localization to performing intracellular concurrent and tandem catalysis together with natural enzymes.

摘要

在生物体系中,特别是在条件下,利用过渡金属催化剂(TMCs)对前药和前荧光团进行生物正交激活仍然是一个挑战。在这里,我们使用了一种介孔有机硅纳米支架(RuMSN),它将 Ru(II) 配合物定位在孔壁上,从而实现了叠氮基团的生物正交光还原反应。由于表面电荷和孔径易于调节,这种高效的工程 RuMSN 催化剂在内部孔井中具有丰富的活性位点,它可以自发排斥或吸引具有不同分子大小和电荷的底物,从而确保选择性的生物正交催化。根据这一点,工程 RuMSN 纳米反应器表现出了从条件性生物正交激活前药和前荧光团,无论是在细胞内还是细胞外定位,到与天然酶一起进行细胞内协同和串联催化的迷人应用规模。

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