Qing Min, Fu Lin, Hu Xuemei, Mu Zhaode, Wu Yijie, Bai Lijuan
Chongqing Research Center for Pharmaceutical Engineering, College of Pharmacy, Chongqing Medical University, Chongqing, 400016, PR China.
Chongqing Research Center for Pharmaceutical Engineering, College of Pharmacy, Chongqing Medical University, Chongqing, 400016, PR China; Department of Respiratory and Critical Care Medicine, the First Affiliated Hospital of Chongqing Medical University, Chongqing, 400016, PR China.
Talanta. 2025 Jun 1;288:127734. doi: 10.1016/j.talanta.2025.127734. Epub 2025 Feb 11.
The development of electrochemiluminescence (ECL) sensors for the sensitive detection of circulating tumor DNA (ctDNA) associated with non-small cell lung cancer (NSCLC) offers a promising approach for early diagnosis; however, the lack of robust and efficient luminophore remains a key limitation to the analytical performance of ECL sensors. Herein, a ECL biosensor is developed using a novel His@ZIF-8/Fe-TCPP (HZTCP) luminophore for the sensitive detection of NSCLC-related ctDNA. The HZTCP luminophore, synthesized using a histidine imidazole framework (His@ZIF-8) as the precursor and tetra-(4-carboxyphenyl) porphyrin ferric chloride (Fe-TCPP) as the luminescent ligand, integrates the photoelectrochemical activity of porphyrin with the porous structure of the MOF, achieving excellent ECL performance. In addition, polyethyleneimine and gold nanoparticle-functionalized covalent organic frameworks (P-COF-AuNPs) serve as interfacial materials to significantly enhance the effective area and conductivity of the sensing interface, increase the solid-state loading of the capture probe, and improve the biosensor's sensitivity. The ECL biosensor achieves a wide detection range of 1 fM to 100 nM with a limit of detection of 0.35 fM, enabling the differentiation of NSCLC patients from healthy individuals through ctDNA detection. This work provides a straightforward approach for designing efficient ECL luminophores and presents a promising method for the rapid detection of non-small cell lung cancer-related ctDNA.
用于灵敏检测与非小细胞肺癌（NSCLC）相关的循环肿瘤DNA（ctDNA）的电化学发光（ECL）传感器的开发为早期诊断提供了一种有前景的方法；然而，缺乏强大而有效的发光体仍然是ECL传感器分析性能的关键限制因素。在此，开发了一种ECL生物传感器，使用新型的His@ZIF-8/Fe-TCPP（HZTCP）发光体来灵敏检测与NSCLC相关的ctDNA。HZTCP发光体以组氨酸咪唑框架（His@ZIF-8）为前体、四（4-羧基苯基）卟啉氯化铁（Fe-TCPP）为发光配体合成，将卟啉的光电化学活性与金属有机框架的多孔结构相结合，实现了优异的ECL性能。此外，聚乙烯亚胺和金纳米颗粒功能化的共价有机框架（P-COF-AuNPs）用作界面材料，可显著提高传感界面的有效面积和电导率，增加捕获探针的固态负载量，并提高生物传感器的灵敏度。该ECL生物传感器实现了1 fM至100 nM的宽检测范围，检测限为0.35 fM，能够通过ctDNA检测区分NSCLC患者和健康个体。这项工作为设计高效的ECL发光体提供了一种直接的方法，并为快速检测与非小细胞肺癌相关的ctDNA提出了一种有前景的方法。
