Department of Analytical Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, China.
Anal Chem. 2021 Nov 30;93(47):15785-15793. doi: 10.1021/acs.analchem.1c04120. Epub 2021 Nov 17.
This work focused on the construction of a nanomaterial-patterned structure for high-resolved ECL signal modulation. Due to the surface coupling effect, the different shapes and distribution states of surface plasmonic nanomaterials not only affect the luminescence intensity enhancement but also decide the electrochemiluminescence (ECL) polarization characteristics. Herein, tin disulfide quantum dots were synthesized via a solvothermal method as ECL emitters. Compared with other nanostructures, Au nanotriangle (Au NT) displayed both the localized surface plasmon resonance electromagnetic enhancement effect and the tip amplification effect, which had significant hot spot regions at three sharp tips. Therefore, self-assembled Au NT-based patterned structures with high density and uniform hot spots were constructed as ideal surface plasmonic materials. More importantly, the distribution states of the hot spots affect the polarization characteristics of ECL, resulting in directional ECL emission at different angles. As a result, a polarization-resolved ECL biosensor was designed to detect miRNA 221. Moreover, this polarization-resolved biosensor achieved good quantitative detection in the linear range of 1 fM to 1 nM and showed satisfactory results in the analysis of the triple-negative breast cancer patients' serum.
本工作致力于构建纳米材料图案结构以实现高分辨率电致化学发光信号调制。由于表面耦合效应,表面等离子体纳米材料的不同形状和分布状态不仅影响发光强度增强,而且决定了电致化学发光(ECL)的偏振特性。在此,通过溶剂热法合成了硫化锡量子点作为 ECL 发射器。与其他纳米结构相比,金纳米三角(Au NT)表现出局域表面等离子体共振电磁增强效应和尖端放大效应,在三个尖锐尖端处具有明显的热点区域。因此,构建了具有高密度和均匀热点的基于自组装 Au NT 的图案结构作为理想的表面等离子体材料。更重要的是,热点的分布状态影响 ECL 的偏振特性,导致在不同角度的定向 ECL 发射。因此,设计了一种偏振分辨 ECL 生物传感器来检测 miRNA 221。此外,这种偏振分辨生物传感器在 1 fM 至 1 nM 的线性范围内实现了良好的定量检测,并在分析三阴性乳腺癌患者的血清时取得了令人满意的结果。