Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing400715, P. R China.
College of Food Science, Chongqing Key Laboratory of Speciality Food Co-Built by Sichuan and Chongqing, Southwest University, Chongqing400715, P. R. China.
Anal Chem. 2023 Feb 14;95(6):3452-3459. doi: 10.1021/acs.analchem.2c05209. Epub 2023 Jan 31.
Herein, the aggregation-induced emission (AIE)-type carboxymethyl chitosan (CMCS)@6-aza-2-thiothymine (ATT) templated AgAu bimetallic nanoclusters (CMCS@ATT-AgAu BMNCs) with superior electrochemiluminescence (ECL) emission were first synthesized to construct a biosensor for the ultrasensitive detection of glial fibrillary acidic protein (GFAP). Impressively, unlike the traditional AIE-type bimetallic nanoclusters (BMNCs) obtained by complicated multi-step synthesis, the AIE-type CMCS@ATT-AgAu BMNCs were prepared by the electrostatic interaction between the negatively charged ATT and positively charged CMCS, in which the molecule ATT was served as a capping and reducing agent of bimetal ions. In addition, a rapidly moving cholesterol labeled DNA walker was constructed to move freely on the lipid bilayer to increase its moving efficiency, and the well-regulated DNA was intelligently designed to further improve its walking efficiency for rapid and ultrasensitive detection of GFAP with a limit of detection (LOD) as low as 73 ag/mL. This strategy proposed an avenue to synthesize highly efficient BMNCs-based ECL emitters, which have great potential in ultrasensitive biosensing for early diagnosis of diseases.
本文首次合成了具有优异电致化学发光（ECL）发射性能的聚集诱导发光（AIE）型羧甲基壳聚糖（CMCS）@6-氮杂-2-硫代胸腺嘧啶（ATT）模板 AgAu 双金属纳米团簇（CMCS@ATT-AgAu BMNCs），用于构建用于检测神经胶质纤维酸性蛋白（GFAP）的超灵敏生物传感器。令人印象深刻的是，与通过复杂的多步合成获得的传统 AIE 型双金属纳米团簇（BMNCs）不同，AIE 型 CMCS@ATT-AgAu BMNCs 通过带负电荷的 ATT 和带正电荷的 CMCS 之间的静电相互作用制备，其中分子 ATT 用作双金属离子的封端和还原剂。此外，构建了一种快速移动的胆固醇标记 DNA walker，使其能够在脂质双层上自由移动，以提高其移动效率，并智能设计了规则的 DNA，以进一步提高其行走效率，从而实现对 GFAP 的快速和超灵敏检测，检测限（LOD）低至 73 ag/mL。该策略为合成基于高效 BMNCs 的 ECL 发射器提供了一种途径，在疾病的早期诊断中用于超灵敏生物传感具有很大的潜力。
