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核心技术专利:CN118964589B侵权必究
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一种基于 MOF 纳米酶介导的串联催化的智能比率荧光分析方法,通过相反逻辑电路指导,用于高灵敏度肌氨酸检测和基于智能手机的便携式传感应用。

An intelligent ratiometric fluorescent assay based on MOF nanozyme-mediated tandem catalysis that guided by contrary logic circuit for highly sensitive sarcosine detection and smartphone-based portable sensing application.

机构信息

Laboratory for Marine Drugs and Bioproducts, National Laboratory for Marine Science and Technology, Key Laboratory of Marine Drugs, Ministry of Education, School of Medicine and Pharmacy, Ocean University of China, Qingdao, Shandong, 266003, China.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China; Intelligent Wearable Engineering Research Center of Qingdao, Research Center for Intelligent and Wearable Technology, College of Textiles and Clothing, State Key Laboratory of Bio-Fibers and Eco-Textiles, Qingdao University, Qingdao, 266071, China.

出版信息

Biosens Bioelectron. 2024 Apr 1;249:116035. doi: 10.1016/j.bios.2024.116035. Epub 2024 Jan 14.


DOI:10.1016/j.bios.2024.116035
PMID:38244294
Abstract

As the well-known test-indicator for early prostate cancer (PCa), sarcosine (SA) is closely related to the differential pathological process, which makes its accurate determination increasingly significant. Herein, we for the first time expanded the peroxidase (POD)-like property of facile-synthesized Zn-TCPP(Fe) MOF to fluorescent substrates and exploited it to ratiometric fluorescent (RF) sensing. By harnessing the effective catalytic oxidation of MOF nanozyme toward two fluorescent substrates (Scopoletin, SC; Amplex Red, AR) with contrary changes, and target-responsive (SA + SOx)/MOF/(SC + AR) tandem catalytic reaction, we constructed the first MOF nanozyme-based RF sensor for the quantitative determination of SA. Superior to previous works, the operation of this RF sensor is under the guidance of AND-(AND^NAND) contrary logic circuit. The dual-channel binary output changes (from 1/0 to 0/1) not only enable the intelligent logical recognition of SA, bringing strengthened reliability and accuracy, but also manifest the proof-of-concept discrimination of PCa individuals and healthy ones. Through recording the fluorescence alterations of SC (F) and AR (F), two segments of linear relationships between ratiometric values (F/F) and varied contents of SA are realized successfully. The LOD for SA could reach to as low as 39.98 nM, which outperforms all nanozyme-originated SA sensors reported till now. Moreover, this sensor also demonstrates high selectivity and satisfactory performance in human serum samples. Furthermore, the portable sensing of SA is realized under the assistance of smartphone-based RGB analysis, demonstrating the potential of point-of-care diagnostics of PCa in the future.

摘要

作为早期前列腺癌 (PCa) 的知名检测指标,肌氨酸 (SA) 与肿瘤的病理过程密切相关,因此对其进行准确的检测变得愈发重要。在此,我们首次扩展了易于合成的 Zn-TCPP(Fe) MOF 的过氧化物酶 (POD) 样特性,将其应用于比率荧光 (RF) 传感。通过利用 MOF 纳米酶对两种荧光底物 (Scopoletin,SC;Amplex Red,AR) 的有效催化氧化作用,以及目标响应 (SA+SOx)/MOF/(SC+AR) 串联催化反应,我们构建了第一个基于 MOF 纳米酶的 RF 传感器,用于定量检测 SA。与之前的工作相比,该 RF 传感器的操作是在与非-(与非^与非)相反逻辑电路的指导下进行的。双通道二进制输出变化 (从 1/0 变为 0/1) 不仅使 SA 的智能逻辑识别成为可能,提高了可靠性和准确性,而且还证明了区分 PCa 个体和健康个体的概念验证能力。通过记录 SC (F) 和 AR (F) 的荧光变化,成功实现了两种不同的比值 (F/F) 值与变化的 SA 含量之间的线性关系。SA 的检测限低至 39.98 nM,优于迄今为止报道的所有基于纳米酶的 SA 传感器。此外,该传感器在人血清样本中也表现出高选择性和良好的性能。此外,在智能手机 RGB 分析的辅助下,实现了 SA 的便携式传感,为未来的 PCa 即时诊断提供了潜力。

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引用本文的文献

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Intelligent nanozymes: Biomimetic design, mechanisms and biomedical applications.

Fundam Res. 2024-12-3

[2]
Catalytic Hairpin Assembly-Propelled Weak-Inputs-Strong-Outputs (CP-WISO) DNA Logic Nanodevices with Orthogonal Design and Contrary Logic Responses.

Adv Sci (Weinh). 2025-9

[3]
Iron-MOFs for Biomedical Applications.

Adv Healthc Mater. 2025-3

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