Chen Jiao-Jie, Qin Ni, Yuan Ruo, Wang Hai-Jun
Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, P. R. China.
Anal Chem. 2025 Jul 8;97(26):14040-14047. doi: 10.1021/acs.analchem.5c02663. Epub 2025 Jun 24.
The environmental contamination caused by deoxynivalenol (DON) has become an emerging public health issue, and its sensitive and accurate analysis is crucial as its trace amounts and microchange in environmental monitoring and management. Here, piperazine-functionalized carbon dot aggregates (P-CDAs) with obvious aggregation-induced electrochemiluminescence (AIECL) properties strengthened by solvent regulation were synthesized, based on which an ECL aptasensor was constructed for the efficient detection of DON. In addition to the surface states optimizing originated from piperazine modification, the aggregation of the P-CDs was further facilitated through solvent regulation, which could directly influence the aggregated process and final ECL performance but was usually neglected in the precious AIECL study. Thus, selecting specific solvents and proportion control was very important for the AIECL. It showed that the P-CDAs could be excited more easily because of the reduced band gap energy and exhibited an improved and red-shifted ECL signal wavelength (603 nm) in ethanol/water (9:1 volume ratio). In addition, to achieve ultrasensitive detection of low-abundance DON, a DNA zipper structure-mediated localized hybridization chain reaction (Z-L-HCR) induced dual-output strategy was constructed. The proposed Z-L-HCR minimized the free diffusion of hairpin DNA, thereby enhancing the reaction rate. Simultaneously, both Z-L-HCR and dual-output mode reduced background signals effectively, realizing the ultrasensitive detection of DON with a detection limit of 0.112 fg/mL. In summary, surface modification and solvent regulation hold significant potential for enhancing the AIECL performance of carbon dots, and the proposed ECL aptasensor provides a reliable detection method for environmental monitoring and food safety.
脱氧雪腐镰刀菌烯醇（DON）造成的环境污染已成为一个新出现的公共卫生问题，由于其在环境监测与管理中的痕量水平及微小变化，对其进行灵敏且准确的分析至关重要。在此，合成了通过溶剂调控强化具有明显聚集诱导电化学发光（AIECL）性质的哌嗪功能化碳点聚集体（P - CDAs），并基于此构建了用于高效检测DON的电化学发光适配体传感器。除了哌嗪修饰带来的表面状态优化外，通过溶剂调控进一步促进了P - CDs的聚集，这可直接影响聚集过程及最终的电化学发光性能，但在以往的AIECL研究中通常被忽视。因此，选择特定溶剂及比例控制对AIECL非常重要。结果表明，由于带隙能量降低，P - CDAs更容易被激发，并且在乙醇/水（体积比9:1）中表现出增强且红移的电化学发光信号波长（603 nm）。此外，为实现对低丰度DON的超灵敏检测，构建了一种DNA拉链结构介导的局部杂交链式反应（Z - L - HCR）诱导双输出策略。所提出的Z - L - HCR使发夹DNA的自由扩散最小化，从而提高了反应速率。同时，Z - L - HCR和双输出模式均有效降低了背景信号，实现了对DON的超灵敏检测，检测限为0.112 fg/mL。总之，表面修饰和溶剂调控在增强碳点的AIECL性能方面具有巨大潜力，所提出的电化学发光适配体传感器为环境监测和食品安全提供了一种可靠的检测方法。
