Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, 400715, Chongqing, People's Republic of China.
Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, School of Materials and Energy and Chongqing Engineering Research Center for Micro-Nano Biomedical Materials and Devices, Southwest University, Chongqing, 400715, People's Republic of China.
Mikrochim Acta. 2023 May 19;190(6):228. doi: 10.1007/s00604-023-05768-1.
Despite black phosphorous (BP) QDs possess the merits of size-tunable band-gap, high electron mobility, and intrinsic defects, the spontaneous agglomeration and rapid oxidation of BP QDs in aqueous solution caused low electrochemiluminescence (ECL) efficiency and unstable ECL signal, which confined its further application of biological analysis. Herein, polyethylene glycol-functionalized BP QDs (PEG@BP QDs) were prepared showing an efficient and stable ECL response, which is attributed to the fact that PEG as protectant not only effectively prevented the spontaneous agglomeration, but also restrained the rapid oxidation of BP QDs in aqueous solution. As proof-of-concept, PEG@BP QDs were used as an efficient ECL emitter to combine with palindrome amplification-induced DNA walker to construct a sensitive ECL aptasensing platform for detecting cancer marker mucin 1 (MUC1). Interestingly, with the aid of positively charged thiolated PEG, the reaction rate of DNA walker on the electrode interface was clearly increased for the recovery of the ECL signal. The ECL aptasensor provides sensitive determination with the detection limit of 16.5 fg/mL. The proposed strategy paves a path for the development of efficient and stable ECL nanomaterials to construct biosensors for biosensing and clinical diagnosis.
尽管黑磷量子点 (BP QDs) 具有可调带隙、高电子迁移率和本征缺陷等优点,但 BP QDs 在水溶液中容易自发聚集和快速氧化,导致其电化学发光 (ECL) 效率低且 ECL 信号不稳定,限制了其在生物分析中的进一步应用。在此,制备了聚乙二醇功能化的 BP QDs(PEG@BP QDs),表现出高效稳定的 ECL 响应,这归因于 PEG 作为保护剂不仅可以有效地防止 BP QDs 的自发聚集,还可以抑制其在水溶液中的快速氧化。作为概念验证,PEG@BP QDs 被用作高效的 ECL 发射器,与回文扩增诱导的 DNA walker 结合,构建了用于检测癌症标志物粘蛋白 1 (MUC1) 的灵敏 ECL 适体传感平台。有趣的是,借助带正电荷的巯基化 PEG,DNA walker 在电极界面上的反应速率明显提高,从而恢复 ECL 信号。该 ECL 适体传感器具有较低的检测限 16.5 fg/mL,提供了灵敏的测定。该策略为开发高效稳定的 ECL 纳米材料以构建用于生物传感和临床诊断的生物传感器铺平了道路。