Zhang Qian, Tian Yu, Liang Zihui, Wang Zizhun, Xu Shuping, Ma Qiang
Department of Analytical Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.
State Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.
Anal Chem. 2021 Feb 16;93(6):3308-3314. doi: 10.1021/acs.analchem.0c05440. Epub 2021 Feb 3.
Herein, we constructed a DNA-mediated Au-Au dimer-based surface plasmon coupling electrochemiluminescence (SPC-ECL) sensor. In the SPC-ECL sensing system, graphite phase carbon nitride quantum dots (GCN QDs) worked as an ECL emitter. A DNA rigid chain structure was employed to connect two Au NPs in an equilateral triangle configuration to form the Au-Au dimers. Due to the hot spot effect, the designed Au-Au dimers had a strong electromagnetic field intensity, which can greatly enhance the ECL signal of GCN QDs than a single Au nanoparticle. The gap distance of dimers can be effectively regulated by the DNA length, which resulted in different electromagnetic field intensities. Therefore, the different SPC-ECL amplification effects on the GCN QD signal by Au-Au dimers have been revealed. The maximum ECL signal of GCN QDs can be enhanced fourfold based on the Au-Au dimers with a gap distance of 2 nm. Furthermore, the biosensor showed good analytical performance for the detection of breast cancer susceptibility gene 1 (BRCA1 genes) (1 fM-1 nM) with a detection limit of 0.83 fM. This work provided an effective and precise SPC-ECL sensing mode for the diagnosis and prognosis of breast cancer.
在此,我们构建了一种基于DNA介导的金-金二聚体的表面等离子体耦合电化学发光(SPC-ECL)传感器。在SPC-ECL传感系统中,石墨相氮化碳量子点(GCN QDs)作为电化学发光发射体。采用DNA刚性链结构将两个金纳米粒子以等边三角形构型连接形成金-金二聚体。由于热点效应,所设计的金-金二聚体具有很强的电磁场强度,与单个金纳米粒子相比,能极大地增强GCN QDs的电化学发光信号。二聚体的间隙距离可通过DNA长度有效调节,这导致了不同的电磁场强度。因此,揭示了金-金二聚体对GCN QD信号的不同SPC-ECL放大效应。基于间隙距离为2 nm的金-金二聚体,GCN QDs的最大电化学发光信号可增强四倍。此外,该生物传感器对乳腺癌易感基因1(BRCA1基因)(1 fM - 1 nM)的检测表现出良好的分析性能,检测限为0.83 fM。这项工作为乳腺癌的诊断和预后提供了一种有效且精确的SPC-ECL传感模式。