Key Laboratory of Bioelectrochemistry and Environmental Analysis of Gansu Province, College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou, 730070, China.
Tianjin Key Laboratory of Molecular Optoelectronic Science, Department of Chemistry, Tianjin University, Tianjin, 300072, P. R. China.
Angew Chem Int Ed Engl. 2019 Apr 23;58(18):5915-5919. doi: 10.1002/anie.201814507. Epub 2019 Mar 27.
Highly efficient detection in the aqueous phase for water-insoluble organic molecule probes is challenging. The bright aggregated-state electrochemiluminescence (ECL) of 1,1-disubstituted 2,3,4,5-tetraphenylsiloles by a co-reactant approach was discovered, and a heterogeneous aggregation-induced emission ECL (HAIE-ECL) was constructed at the electrode surface, showing very high ECL efficiency (37.8 %) and selective recognition for industrially important DNBP plasticizer with a low detection limit of 0.15 nm in the water phase. A mechanistic study indicates that ECL is mainly generated due to the high electron affinity of siloles and restriction of the intramolecular motions caused by their propeller-like noncoplanar structures. This system realizes the sensing of organic-based ECL in the water phase by solving the crucial problems of water insolubility and aggregation-caused quenching (ACQ), and demonstrates potential for further application because of its design and high efficiency.
高效检测水不溶性有机分子探针在水相中的存在具有挑战性。通过共反应物方法发现了 1,1-二取代 2,3,4,5-四苯基硅咯的亮聚集态电化学发光（ECL），并在电极表面构建了非均相聚集诱导发射 ECL（HAIE-ECL），在水相中对工业上重要的邻苯二甲酸二正丁酯增塑剂表现出非常高的 ECL 效率（37.8%）和选择性识别，检测限低至 0.15nm。机理研究表明，ECL 主要是由于硅咯的高电子亲和力和它们的推进器状非共面结构引起的分子内运动受限而产生的。该系统通过解决水不溶性和聚集猝灭（ACQ）这两个关键问题，实现了基于有机的 ECL 在水相中的传感，由于其设计和高效率，展示了进一步应用的潜力。
