Specific Coordination between Zr-MOF and Phosphate-Terminated DNA Coupled with Strand Displacement for the Construction of Reusable and Ultrasensitive Aptasensor

化学 适体 检出限 线性范围 配位复合体 纳米技术 组合化学 色谱法 有机化学 遗传学 生物 材料科学 金属
作者
Weiwei Qiu,Feng Gao,Natsumi Yano,Yosuke Kataoka,Makoto Handa,Weiqiang Yang,Hidekazu Tanaka,Qingxiang Wang
出处
期刊:Analytical Chemistry [American Chemical Society]
卷期号:92 (16): 11332-11340 被引量:56
标识
DOI:10.1021/acs.analchem.0c02018
摘要

Electrochemical aptasensors involved in chemical labeling are often single-use and sensitivity-limited because the probes are commonly single-point labeled and irreversible. In this work, the specific coordination between Zr4+ and phosphate group (−PO43–) was employed to construct a new aptasensor that is highly sensitive and reusable, using Ochratoxin A (OTA) as the test model. The OTA binding aptamer (OBA) was hybridized with the thiolated supporting sequence (TSS) immobilized on the surface of a gold electrode. The UiO-66 with a formula of [Zr6O4(OH)4(BDC)6], one of the class of Zr metal–organic frameworks (MOFs), was then particularly grafted on the terminal of OBA through the specific coordination between Zr4+ and 5′-PO43–, i.e., the Zr–O–P coordination bond. Similarly, as much as the 5′-PO43– and 3′-methylene blue dual-labeled sequences (DLS) were further assembled on UiO-66 due to the large surface area of MOF and rich active sites of Zr4+. Owing to the specific coordination for signal amplification, the developed aptasensor shows greatly enhanced sensitivity. A wide detection range from 0.1 fM to 2.0 μM and an ultralow detection limit of 0.079 fM (S/N = 3) for OTA were obtained. Additionally, the TSS can rehybridize with a new OBA to regenerate the aptasensor but without complicated pretreatments, enabling a aptasensor that is readily reusable for OTA detection. The aptasensor was successfully applied for OTA detection in the red wine samples, demonstrating a promising prospect for food safety monitoring.
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