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基于 Co 的金属有机骨架与银-半胱氨酸的三重放大 3,4,9,10-苝四羧酸及其在降钙素原超灵敏检测中的应用。

Triple Amplification of 3,4,9,10-Perylenetetracarboxylic Acid by Co-Based Metal-Organic Frameworks and Silver-Cysteine and Its Potential Application for Ultrasensitive Assay of Procalcitonin.

机构信息

Collaborative Innovation Center for Green Chemical Manufacturing and Accurate Detection, Key Laboratory of Chemical Sensing & Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering , University of Jinan , Jinan 250022 , P. R. China.

School of Chemical Engineering , Shandong University of Technology , Zibo 255049 , P.R. China.

出版信息

ACS Appl Mater Interfaces. 2020 Feb 26;12(8):9098-9106. doi: 10.1021/acsami.9b23248. Epub 2020 Feb 12.

Abstract

In this work, a triple-amplified biosensor with a bioactivity-maintained peculiarity was constructed for quantitative procalcitonin (PCT) detection. As everyone knows, a strong electrochemiluminescence (ECL) signal is the premise to ensure high sensitivity for trace target detection. Hence, a valid tactic was developed to achieve signal amplification of luminophor by using Co-based metal-organic frameworks (ZIF-67) and silver-cysteine (AgCys). The ZIF-67 particles, which have more atomically dispersed Co, could play the role of a co-reaction accelerator to catalyze SO to generate abundant Co and sulfate radical anions (SO). Afterward, a mass of Co was reduced to more hydroxyl radicals (OH) by HO, thus ulteriorly reducing SO to generate more SO. Remarkably, SO was reduced to SO continuously with the recycling of Co and Co, which realized an effective signal amplification. Meanwhile, the AgCys complex with superior catalysis and biocompatibility was prepared to further improve the ECL signal and maintain the bioactivity of the biomolecule. Furthermore, HWRGWVC, a heptapeptide that was used for combining the Fc fragments of an antibody by Au-S bonding to achieve the fixed point fixation, could not only maintain bioactivity of an antibody but also improved its incubation efficiency, thus further enhancing biosensor sensitivity. Under optimum conditions, the proposed biosensor realized highly sensitive assay for PCT with a wide dynamic range from 10 fg/mL to 100 ng/mL and a detection limit as low as 3.67 fg/mL. With superior stability, selectivity, and repeatability, the prepared biosensor revealed immense potential application of ultrasensitive assay for PCT in human serum.

摘要

在这项工作中,构建了一种具有生物活性保持特性的三重放大生物传感器,用于定量检测降钙素原 (PCT)。众所周知,强电化学发光 (ECL) 信号是确保痕量目标检测高灵敏度的前提。因此,开发了一种有效的策略,通过使用钴基金属-有机骨架 (ZIF-67) 和银-半胱氨酸 (AgCys) 来实现发光体的信号放大。具有更多原子分散 Co 的 ZIF-67 颗粒可以起到共同反应加速剂的作用,以催化 SO 生成丰富的 Co 和硫酸根自由基阴离子 (SO)。之后,大量的 Co 被 HO 还原为更多的羟基自由基 (OH),从而进一步将 SO 还原为更多的 SO。值得注意的是,SO 通过 Co 和 Co 的循环不断被还原为 SO,实现了有效的信号放大。同时,制备了具有优异催化性和生物相容性的 AgCys 配合物,以进一步提高 ECL 信号并保持生物分子的生物活性。此外,HWRGWVC 是一种七肽,通过 Au-S 键将抗体的 Fc 片段结合起来实现定点固定,不仅可以保持抗体的生物活性,还可以提高其孵育效率,从而进一步提高生物传感器的灵敏度。在最佳条件下,所提出的生物传感器实现了对 PCT 的高灵敏度检测,具有从 10 fg/mL 到 100 ng/mL 的宽动态范围和低至 3.67 fg/mL 的检测限。该制备的生物传感器具有优异的稳定性、选择性和可重复性,在人血清中超敏检测 PCT 方面具有巨大的潜在应用价值。

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