双金属片
辣根过氧化物酶
催化作用
葡萄糖氧化酶
材料科学
组合化学
金属有机骨架
级联反应
过氧化物酶
生物传感器
金属
反应速率常数
化学工程
化学
动力学
纳米技术
有机化学
酶
吸附
工程类
物理
量子力学
冶金
作者
Qiaoshi Jiang,Yuchen Xiao,Anh N. Hong,Ziting Gao,Yuyang Shen,Qingsong Fan,Pingyun Feng,Wenwan Zhong
标识
DOI:10.1021/acsami.2c12115
摘要
Metal-organic frameworks (MOFs) have many attractive features, including tunable composition, rigid structure, controllable pore size, and large specific surface area, and thus are highly applicable in molecular analysis. Depending on the MOF structure, a high number of unsaturated metal sites can be exposed to catalyze chemical reactions. In the present work, we report that using both Co(II) and Fe(III) to prepare the MIL-88(NH2) MOF, we can produce the bimetallic MOF that can catalyze the conversion of 3,3',5,5″-tetramethylbenzidine (TMB) to a color product through a reaction with H2O2 at a higher reaction rate than the monometallic Fe-MIL-88(NH2). The Michaelis constants (Km) of the catalytic reaction for TMB and H2O2 are 3-5 times smaller, and the catalytic constants (kcat) are 5-10 times higher than those of the horseradish peroxidase (HRP), supporting ultrahigh peroxidase-like activity. These values are also much more superior to those of the HRP-mimicking MOFs reported previously. Interestingly, the bimetallic MOF can be coupled with glucose oxidase (GOx) to trigger the cascade enzymatic reaction for highly sensitive detection of extracellular vesicles (EVs), a family of important biomarkers. Through conjugation to the aptamer that recognizes the marker protein on EV surface, the MOF can help isolate the EVs from biological matrices, which are subsequently labeled by GOx via antibody recognition. The cascade enzymatic reaction between MOF and GOx enables the detection of EVs at a concentration as low as 7.8 × 104 particles/mL. The assay can be applied to monitor EV secretion by cultured cells and also can successfully detect the different EV quantities in the sera samples collected from cancer patients and healthy controls. Overall, we prove that the bimetallic Fe/Co-MIL-88(NH2) MOF, with its high peroxidase activity and high biocompatibility, is a valuable tool deployable in clinical assays to facilitate disease diagnosis and prognosis.
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