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一种以MOF-on-MOF衍生电催化剂作为信号放大器的磁性双适体电化学传感器,用于灵敏检测心肌肌钙蛋白I。

A magnetic dual-aptamer electrochemical sensor with MOF-on-MOF-derived electrocatalyst as a signal amplifier for sensitive detection of cardiac troponin I.

作者信息

Peng Xiaolun, Xu Ruijie, Yu Fan, Xu Junhui, Wang Yazhen, Wang Shengfu

机构信息

Key Laboratory of Optoelectronic Chemical Materials and Devices of Ministry of Education, College of Optoelectronic Materials and Technology, Jianghan University, 430056, Wuhan, China.

Key Laboratory of Optoelectronic Chemical Materials and Devices of Ministry of Education, College of Optoelectronic Materials and Technology, Jianghan University, 430056, Wuhan, China.

出版信息

Talanta. 2025 Feb 1;283:127177. doi: 10.1016/j.talanta.2024.127177. Epub 2024 Nov 12.

Abstract

Considering the close association between cardiac troponin I (cTnI) level and various cardiovascular diseases, it becomes essential to explore sensitive and accurate detection methods for monitoring their levels in the early stages of disease. In this work, a magnetic dual-aptamer electrochemical sensor for cTnI detection was constructed in the first utilizing MOF-on-MOF-derived electrocatalyst as a signal amplifier in collaboration with high-efficient separation of magnetic beads (MBs). Employing zeolitic imidazolate framework-67 (ZIF-67) with high surface area as host MOF, MOF-on-MOF heterostructure (ZIF-67@PBA) was facilely prepared by in-situ growth of conductive prussian blue analogue (PBA) as guest MOF onto the surface of ZIF-67 with a simple ion-exchange method. After low-temperature calcination, N doped derived electrocatalyst (N-ZIF-67@PBA) was obtained with intact skeletons and pore structures of MOFs. This not only integrated bimetallic active centers with various valence states and diversiform nanostructures of dual MOF, but endowed N-ZIF-67@PBA 8.3-fold increase of electrocatalytic activity for catalytic amplification. Further using aptamer-modified MBs as capture carriers for recognizing and separating cTnI from complex samples with high specificity, the magnetic dual-aptamer sensor successfully achieved the sensitive detection of cTnI with a low detection limit of 0.31 fg/mL. This work provided a new viewpoint on the use of MOF-on-MOF-derived electrocatalyst for ultrasensitive electrochemical sensing analysis.

摘要

鉴于心肌肌钙蛋白I(cTnI)水平与各种心血管疾病之间的密切关联,探索灵敏且准确的检测方法以在疾病早期监测其水平变得至关重要。在这项工作中,首先构建了一种用于检测cTnI的磁性双适配体电化学传感器,该传感器利用MOF-on-MOF衍生的电催化剂作为信号放大器,并结合磁珠(MBs)的高效分离。以具有高比表面积的沸石咪唑酯骨架-67(ZIF-67)作为主体MOF,通过简单的离子交换方法将导电普鲁士蓝类似物(PBA)作为客体MOF原位生长在ZIF-67表面,轻松制备了MOF-on-MOF异质结构(ZIF-67@PBA)。经过低温煅烧,获得了具有完整MOF骨架和孔结构的N掺杂衍生电催化剂(N-ZIF-67@PBA)。这不仅整合了具有多种价态和双MOF多样纳米结构的双金属活性中心,还使N-ZIF-67@PBA的电催化活性提高了8.3倍以进行催化放大。进一步使用适配体修饰的磁珠作为捕获载体,以高特异性从复杂样品中识别和分离cTnI,该磁性双适配体传感器成功实现了对cTnI的灵敏检测,检测限低至0.31 fg/mL。这项工作为使用MOF-on-MOF衍生的电催化剂进行超灵敏电化学传感分析提供了新的视角。

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