State Key Laboratory for Food Nutrition and Safety; College of Food Engineering and Biotechnology, Tianjin University of Science and Technology, Tianjin 300457, China.
State Key Laboratory for Food Nutrition and Safety; College of Food Engineering and Biotechnology, Tianjin University of Science and Technology, Tianjin 300457, China.
Biosens Bioelectron. 2019 Mar 1;128:129-136. doi: 10.1016/j.bios.2018.12.043. Epub 2018 Dec 27.
For the determination of dopamine (DA) in serum samples, a quenching-type electrochemiluminescence sensor (MIECLS) was constructed in this study. Upconversion nanoparticles (UCNPs) enhanced by covalent organic frameworks (COFs)-based hybrid and oligoaniline-crosslinked gold nanoparticles (AuNPs) imprinting recognition sites were introduced in electrochemiluminescence (ECL) system at the first time. The porous COFs-based hybrid with large specific surface area was modified on the electrode firstly to hold more UCNPs and imprinting recognition sites. AuNPs was employed in the developed sensor for two objectives: 1) AuNPs on the COFs-based hybrid enabled the hybrid to tunnel the electrons, which helped to improve the ECL intensity; 2) AuNPs-based thioaniline units (PATP@AuNPs) electropolymerized on the electrode in the presence of template to form oligoaniline-crosslinked AuNPs matrix. Then the exclusion of template from matrix yielded the molecularly three-dimensional imprinted contours with conductivity, which facilitated specific recognition and further amplified the ECL. The double recognition mode in this work involves the recognition effect of imprinted contours and quenching effect of o-benzoquinone species. The quantum chemical calculation was performed to analyze the possible recognition and the binding mechanisms of molecularly three-dimensional imprinted contours. The results showed imprinted contours could bind the targets by complementary spatial cavities and weak interactions. The proposed approach yielded a wide detection range (10-10 M), low limit of detection (LOD = 2 ×10 M) and acceptable recoveries (93.25-112.97%) in rat serum sample, demonstrating that the developed method holds great promise to be applied to DA detection in practical samples.
为了测定血清样本中的多巴胺（DA），本研究构建了一种猝灭型电化学发光传感器（MIECLS）。首次在电化学发光（ECL）体系中引入了基于共价有机框架（COFs）的杂化和聚邻苯二胺交联金纳米粒子（AuNPs）增强的上转换纳米粒子（UCNPs）印迹识别位点。首先在电极上修饰具有大比表面积的多孔 COFs 基杂化材料，以容纳更多的 UCNPs 和印迹识别位点。AuNPs 被用于开发的传感器中，有两个目的：1）COFs 基杂化材料上的 AuNPs 使杂化材料能够隧穿电子，这有助于提高 ECL 强度；2）在模板存在的情况下，AuNPs 上的硫代苯胺单元（PATP@AuNPs）在电极上电聚合形成聚邻苯二胺交联的 AuNPs 基质。然后，模板从基质中排除，得到具有导电性的分子三维印迹轮廓，这有利于特异性识别，并进一步放大 ECL。本工作中的双识别模式涉及印迹轮廓的识别效应和邻苯醌物种的猝灭效应。进行了量子化学计算，以分析分子三维印迹轮廓的可能识别和结合机制。结果表明，印迹轮廓可以通过互补的空间腔和弱相互作用结合靶标。所提出的方法在大鼠血清样品中表现出较宽的检测范围（10-10 M）、低检测限（LOD=2×10 M）和可接受的回收率（93.25-112.97%），表明该方法在实际样品中检测 DA 具有很大的应用前景。
