Liu Lipeng, Chen Wenze, Yin Lu, Sun Xiaojun, Li Yan, Wei Qin, Ma Hongmin
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, PR China.
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, PR China; Department of Chemistry, Sungkyunkwan University, Suwon, 16419, Republic of Korea.
Biosens Bioelectron. 2025 Dec 15;290:118013. doi: 10.1016/j.bios.2025.118013. Epub 2025 Sep 19.
Early screening for breast cancer can be effective in reducing cancer mortality; therefore, accurate detection of breast cancer marker carbohydrate antigen 15-3 (CA15-3) is of great importance. In this study, a highly sensitive sandwich-type electrochemiluminescence (ECL) biosensor based on an electron transfer quenching mechanism was developed for the ultrasensitive detection of the CA15-3. The self-assembled biohybrid framework through hydrogen bonding between the amino groups (-NH) of bovine serum albumin (BSA) and the carboxylic acid groups (-COOH) of perylene tetracarboxylic acid (PTCA) was used as a luminophore. The aggregation-caused quenching (ACQ) effect was effectively suppressed by framework spatial arrangement preventing PTCA aggregation and enhancing ECL emission. Simultaneously, introduction of Au NCs with BSA as a protective ligand catalyzed the production of more SO radicals from SO to enhance ECL emission intensity. CuO@MnO with matched energy level can be used as an electron transfer quencher to construct sandwich-type ECL biosensors. ECL signals was quenched by target response via the electron transfer (ET) pathway. The sensor achieves sensitive detection of CA15-3 under optimal conditions with a wide response range (0.001-100 U/mL) and a low limit of detection (LOD) (0.00014 U/mL), and has sufficient practical analytical performance. This study provides a high-precision analytical platform for the sensitive detection of CA15-3 and offers more possibilities for the development of ECL systems based on novel biohybridisation frameworks.
早期乳腺癌筛查可有效降低癌症死亡率；因此，准确检测乳腺癌标志物糖类抗原15-3（CA15-3）至关重要。在本研究中，基于电子转移猝灭机制开发了一种高灵敏度的夹心型电化学发光（ECL）生物传感器，用于超灵敏检测CA15-3。通过牛血清白蛋白（BSA）的氨基（-NH）与苝四羧酸（PTCA）的羧酸基团（-COOH）之间的氢键作用形成的自组装生物杂交框架用作发光体。通过框架空间排列有效抑制了聚集诱导猝灭（ACQ）效应，防止PTCA聚集并增强ECL发射。同时，引入以BSA为保护配体的金纳米簇催化从SO产生更多的SO自由基以增强ECL发射强度。具有匹配能级的CuO@MnO可作为电子转移猝灭剂来构建夹心型ECL生物传感器。通过电子转移（ET）途径，目标响应使ECL信号猝灭。该传感器在最佳条件下实现了对CA15-3的灵敏检测，具有宽响应范围（0.001-100 U/mL）和低检测限（LOD）（0.00014 U/mL），并具有足够的实际分析性能。本研究为CA15-3的灵敏检测提供了一个高精度分析平台，并为基于新型生物杂交框架的ECL系统开发提供了更多可能性。
