<br>双功能 TiO2 纳米花诱导的 H4TCBPE 聚集增强电化学发光用于有机磷的超灵敏测定,Analytical Chemistry

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双功能 TiO2 纳米花诱导的 H4TCBPE 聚集增强电化学发光用于有机磷的超灵敏测定
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-11-16 , DOI: 10.1021/acs.analchem.3c04183
Jiao Qin ₁ , Jinjin Li ₁ , Haisen Zeng ₁ , Fan Du ₁ , Dianping Tang ₂ , Juan Tang ₁

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在这项工作中，聚集诱导发射配体1,1,2,2-四(4-羧基联苯)乙烯(H ₄ TCBPE)在Ti-O网络中被刚性化，形成新型电化学发光(ECL)发射体H ₄ TCBPE- TiO ₂纳米球作为有效的 ECL 发射器构建了“开关”ECL 生物传感器，用于超灵敏检测马拉硫磷 (Mal)。由于Ti-O网络可以限制H ₄ TCBPE内的分子内自由运动，从而减少非辐射弛豫，H ₄ TCBPE-TiO ₂表现出优异的ECL响应。此外，TiO ₂可以作为ECL共反应促进剂，促进硫酸根阴离子（SO ₄ ^•– ）的产生，其与Ti-O网络中的H ₄ TCBPE相互作用，产生增强的ECL响应。在 Mal 存在的情况下，通过无铜点击核酸连接反应形成并释放大量连接探针（探针 1 至探针 2，P1–P2），然后与发夹探针 1 (H1) 修饰的 H ₄ TCBPE- 杂交。 TiO ₂基电极表面。 P1-P2探针可以启动靶向辅助末端脱氧核苷转移酶（TdTase）延伸反应，产生含有丰富生物素的长尾脱氧腺嘌呤，可以负载大量链霉亲和素功能化二茂铁二甲酸聚合物（SA-PFc），导致ECL猝灭信号。因此，基于H ₄ TCBPE-TiO ₂ ECL发射器和点击化学驱动的TdTase放大策略的超灵敏ECL生物传感器呈现出0.001至100ng/mL的理想范围和低至9.9fg/mL的检测限。总体而言，这项工作为新型 ECL 发射器的开发铺平了道路，为 ECL 生物传感开辟了新的前景。

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Bifunctional TiO2 Nanoflower-Induced H4TCBPE Aggregation Enhanced Electrochemiluminescence for an Ultrasensitive Assay of Organophosphorus

In this work, the aggregation-induced emission ligand 1,1,2,2-tetra(4-carboxylbiphenyl)ethylene (H₄TCBPE) was rigidified in the Ti–O network to form novel electrochemiluminescence (ECL) emitter H₄TCBPE-TiO₂ nanospheres, which acted as an effective ECL emitter to construct an “on–off” ECL biosensor for ultrasensitive detection of malathion (Mal). H₄TCBPE-TiO₂ exhibited excellent ECL responses due to the Ti–O network that can restrict the intramolecular free motions within H₄TCBPE and then reduce the nonradiative relaxation. Moreover, TiO₂ can act as an ECL co-reaction accelerator to promote the generation of sulfate radical anion (SO₄^•–), which interacts with H₄TCBPE in the Ti–O network to produce enhanced ECL response. In the presence of Mal, numerous ligated probes (probe 1 to probe 2, P1–P2) were formed and released by copper-free click nucleic acid ligation reaction, which then hybridized with hairpin probe 1 (H1)-modified H₄TCBPE-TiO₂-based electrode surface. The P1–P2 probes can initiate the target-assisted terminal deoxynucleoside transferase (TdTase) extended reaction to produce long tails of deoxyadenine with abundant biotin, which can load numerous streptavidin-functionalized ferrocenedicarboxylic acid polymer (SA-PFc), causing quenching of the ECL signal. Thus, the ultrasensitive ECL biosensor based on H₄TCBPE-TiO₂ ECL emitter and click chemistry-actuated TdTase amplification strategy presents a desirable range from 0.001 to 100 ng/mL and a detection limit low to 9.9 fg/mL. Overall, this work has paved an avenue for the development of novel ECL emitters, which has opened up new prospects for ECL biosensing.

更新日期：2023-11-16

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