Abstract：
Recognition and separation of chiral isomers are of great importance in both industrial and biological applications. However, owing to identical molecular formulas and chemical properties of enantiomers, signal transduction and amplification are still two major challenges in chiral sensing. In this study, we developed an enantioselective device by integrating chiral covalent organic framework nanosheets (CONs) with nanochannels for sensitive identification and quantification of enantiomers. Using 3,4-dihydroxyphenylalanine (DOPA) as the model analyte, the as-prepared chiral nanofluidic device exhibits a remarkable chiral recognition ability to l-DOPA than d-DOPA. More importantly, due to the chelation of DOPA with Fe3+ ions, it can efficiently block the ion transport through channel and shield the channel surface charge, which will amplify the difference in the electrochemical response of l-DOPA and d-DOPA. Therefore, a sensitive chiral recognition can be achieved using the present nanofluidic device coupled using electrochemical amplification strategy. Notably, using this method, an ultra-low concentration of l-DOPA (as low as 0.21 pM) can be facilely and successfully detected with a linear range of 1 pM-10 μM. This study provides a reliable and sensitive approach for achieving highly selective detection of chiral molecules.
摘要：
手性异构体的识别和分离在工业和生物应用中都非常重要。然而,由于对映体的分子式和化学性质相同，信号转导和放大仍然是手性传感的两大挑战。在这项研究中,我们通过将手性共价有机骨架纳米片（CONs）与纳米通道集成，开发了一种对映选择性装置，用于对对映异构体的灵敏鉴定和定量。使用3,4-二羟基苯丙氨酸（DOPA）作为模型分析物，与d-DOPA相比，所制备的手性纳米流体装置对l-DOPA具有显着的手性识别能力。更重要的是,由于DOPA与Fe3+离子螯合，它可以有效地阻止离子通过通道传输并屏蔽通道表面电荷，这将放大l-DOPA和d-DOPA的电化学响应的差异。因此,灵敏的手性识别可以使用本发明的使用电化学放大策略耦合的纳米流体装置来实现。值得注意的是,使用这种方法，可以在1pM-10μM的线性范围内轻松成功地检测到超低浓度的1-DOPA（低至0.21pM）。本研究为实现手性分子的高选择性检测提供了一种可靠而灵敏的方法。
