Sun Ruifen, Xiong Shuyun, Zhang Weiwei, Huang Yun, Zheng Jingcheng, Shao Jiwei, Chi Yuwu
MOE Key Laboratory for Analytical Science of Food Safety and Biology, Fujian Provincial Key Laboratory of Analysis and Detection for Food Safety, College of Chemistry, Fuzhou University, Fuzhou, Fujian 350108, China.
Anal Chem. 2024 Apr 9;96(14):5711-5718. doi: 10.1021/acs.analchem.4c00951. Epub 2024 Mar 29.
Self-enhanced electrochemiluminescence (ECL) probes have attracted more and more attention in analytical chemistry for their significant simplification of the ECL sensing operation while improving the ECL sensing sensitivity. However, the development and applications of self-enhanced ECL probes are still in their infancy and mainly suffer from the requirement of a complicated synthesis strategy and relatively low self-enhanced ECL activity. In this work, we took advantage of the recently emerged perovskite quantum dots (PQDs) with high optical quantum yields and easy surface engineering to develop a new type of PQD-based self-enhanced ECL system. The long alkyl chain (C) diethanolamine (i.e., -octadecyldiethanolamine (ODA)) with high ECL coreactant activity was selected as a capping ligand to synthesize an ODA-capped PQD self-enhanced ECL probe. The preparation of the coreactant-capped PQDs is as simple as for the ordinary oleylamine (OAm)-capped PQDs, and the obtained ODA-capped PQDs exhibit very strong self-enhanced ECL activity, 82.5 times higher than that of traditional OAm-capped PQDs. Furthermore, the prepared ODA-PQDs have a unique nanostructure (ODA-CsPbBr@CsPbBr), with the highly emissive 3D CsPbBr PQD as the core and the water-stable 2D CsPbBr as the shell, which allows ODA-PQDs to be very stable in aqueous media. It is envisioned that the prepared ODA-3D@2D PQDs with the easy preparation method, strong self-enhanced ECL, and excellent water stability have promising applications in ECL sensing.
自增强电化学发光（ECL）探针在分析化学中受到越来越多的关注，因为它们显著简化了ECL传感操作，同时提高了ECL传感灵敏度。然而，自增强ECL探针的开发和应用仍处于起步阶段，主要受制于复杂的合成策略要求以及相对较低的自增强ECL活性。在这项工作中，我们利用最近出现的具有高光学量子产率且易于进行表面工程的钙钛矿量子点（PQD）来开发一种新型的基于PQD的自增强ECL系统。选择具有高ECL共反应剂活性的长烷基链（C）二乙醇胺（即十八烷基二乙醇胺（ODA））作为封端配体，合成了ODA封端的PQD自增强ECL探针。制备共反应剂封端的PQD与制备普通油胺（OAm）封端的PQD一样简单，并且所获得的ODA封端的PQD表现出非常强的自增强ECL活性，比传统的OAm封端的PQD高82.5倍。此外，制备的ODA-PQD具有独特的纳米结构（ODA-CsPbBr@CsPbBr），以高发射性的3D CsPbBr PQD为核心，水稳定的2D CsPbBr为壳层，这使得ODA-PQD在水性介质中非常稳定。可以预见，所制备的具有易于制备方法、强自增强ECL和优异水稳定性的ODA-3D@2D PQD在ECL传感方面具有广阔的应用前景。
