Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Ministryof Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules&College of Chemistry and Chemical Engineering, Hubei University, Wuhan 430062, China.
Nanoscale. 2019 Sep 19;11(36):16860-16867. doi: 10.1039/c9nr02190f.
Electrochemiluminescence (ECL) nanomaterials are usually deposited compactly on the surface of electrodes, which may cause poor mass transfer of reactants, thereby resulting in low ECL efficiency. In this work, we developed a novel kind of luminescent material denoted as C-Au-luminol nanospheres (C-Au-Lum NSs) by high dispersion of luminophores on porous carbon nanospheres (PCNSs). C-Au-Lum NSs were facilely prepared by the in situ reduction of chloroauric acid with the luminescent reagent luminol (Lum) on the nano-pores of PCNSs. Plenty of luminescent Au-Lum NPs were dispersedly concentrated inside the numerous pores and hollow interiors of PCNSs, effectively increasing the mass transfer of reagents and accelerating the electron transport inside the porous nanospheres. This greatly improved the availability of luminophores and endowed C-Au-Lum NSs with excellent ECL emission. After further integrating with enzymatic circulation and strand displacement, an ultrasensitive ECL biosensor was achieved for the ultrasensitive detection of an important tumor biomarker, mucin1. The logarithmically linear range from 0.1 pg mL-1 to 1 ng mL-1 with the detection limit of 47.6 fg mL-1 (S/N = 3) was achieved, demonstrating the superior performance of C-Au-Lum NSs. This work would provide new ideas for the construction of high-performance ECL sensing platforms for diverse applications.
电致化学发光（ECL）纳米材料通常紧密沉积在电极表面上，这可能导致反应物的传质不良，从而导致 ECL 效率低下。在这项工作中，我们通过将发光体高度分散在多孔碳纳米球（PCNSs）上，开发了一种新型发光材料，记为 C-Au-鲁米诺纳米球（C-Au-Lum NSs）。C-Au-Lum NSs 通过氯金酸与发光试剂鲁米诺（Lum）在 PCNSs 的纳米孔原位还原来简便制备。大量发光的 Au-Lum NPs 分散在 PCNSs 的众多孔和中空内部集中，有效地增加了试剂的传质并加速了多孔纳米球内的电子传递。这极大地提高了发光体的利用率，并赋予 C-Au-Lum NSs 优异的 ECL 发射性能。进一步与酶循环和链置换相结合，实现了用于检测重要肿瘤生物标志物粘蛋白 1 的超灵敏 ECL 生物传感器。实现了从 0.1 pg mL-1 到 1 ng mL-1 的对数线性范围，检测限为 47.6 fg mL-1（S/N = 3），证明了 C-Au-Lum NSs 的优越性能。这项工作将为构建用于各种应用的高性能 ECL 传感平台提供新的思路。
