Du Yu, Jiang Su, Han Yun, Liu Qian, Cui Lin, Zhang Chun-Yang
College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan, 250014, China.
School of Chemistry and Chemical Engineering, Southeast University, Nanjing, 211189, China.
Talanta. 2024 May 15;272:125752. doi: 10.1016/j.talanta.2024.125752. Epub 2024 Feb 10.
The reported organic electrochemiluminescence (ECL) luminophors for the detection of various markers often suffer from intermolecular π-π stacking-induced luminophore quenching. Herein, we demonstrate one-pot synthesis of a new aggregation-induced electrochemiluminescence (AIECL) emitter (i.e., TPE@SiO/rGO composite) for sensitive measurement of microcystin-leucine arginine (MC-LR). The TPE@SiO/rGO composite is constructed by embedding the silica-encapsuled 1,1,2,2-tetra(4-carboxylphenyl)ethylene (TPE) in the reduced graphene oxide. In comparison with the monomer TPE, this composite exhibit high luminescence efficiency and strong ECL emission, because the AIECL phenomenon triggered by the spatial confinement effect in the SiO cage induces the restriction of the internal motion and vibration of molecules. Notably, this composite has distinct advantages of easy preparation, simple functionalization, and stable luminescence. Especially, the TPE@SiO/rGO-based ECL-RET system exhibits a high quenching efficiency (Φ) of 69.7%. When target MC-LR is present, it triggers DNA strand displacement reaction (SDR), inducing the quenching of the ECL signal of TPE@SiO/rGO composite due to ECL resonance energy transfer between TPE@SiO/rGO composite and methylene blue (MB). The proposed biosensor enables highly sensitive, low-cost, and robust measurement of MC-LR with a large dynamic range of 7 orders of magnitude and a detection limit of 3.78 fg/mL, and it displays excellent detection performance in complex biological matrices, holding potential applications in food safety and water monitoring.
据报道，用于检测各种标志物的有机电化学发光（ECL）发光体常常受到分子间π-π堆积诱导的发光体猝灭的影响。在此，我们展示了一种用于灵敏检测微囊藻毒素-亮氨酸-精氨酸（MC-LR）的新型聚集诱导电化学发光（AIECL）发光体（即TPE@SiO/rGO复合材料）的一锅法合成。TPE@SiO/rGO复合材料是通过将二氧化硅包裹的1,1,2,2-四（4-羧基苯基）乙烯（TPE）嵌入还原氧化石墨烯中构建而成。与单体TPE相比，该复合材料表现出高发光效率和强ECL发射，这是因为SiO笼中的空间限制效应引发的AIECL现象导致分子内部运动和振动受到限制。值得注意的是，这种复合材料具有制备简便、功能化简单和发光稳定的明显优势。特别是，基于TPE@SiO/rGO的ECL-RET系统表现出69.7%的高猝灭效率（Φ）。当存在目标MC-LR时，它引发DNA链置换反应（SDR），由于TPE@SiO/rGO复合材料与亚甲基蓝（MB）之间的ECL共振能量转移，导致TPE@SiO/rGO复合材料的ECL信号猝灭。所提出的生物传感器能够对MC-LR进行高灵敏、低成本且稳健的测量，动态范围达7个数量级，检测限为3.78 fg/mL，并且在复杂生物基质中显示出优异的检测性能，在食品安全和水质监测方面具有潜在应用价值。
