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同时操控竞争机制以构建基于谷胱甘肽稳定的金纳米簇的双通道分子分类器用于金属离子检测和信息隐写术。

Concurrent manipulation of competitive mechanisms to construct glutathione-stabilized gold nanocluster-based dual-channel molecular classifier for metal ions detection and information steganography.

作者信息

Li Na, Long Qing-Hong, Li Xin-Yuan, Dong Can, Zhao Tian-Sheng, Mai Xi, Zhao Yong-Sen, Gao Zhong-Feng, Wei Qin, Xia Fan

机构信息

School of Pharmaceutical Science, Nanchang University, Nanchang, 330006, PR China.

Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, PR China.

出版信息

Talanta. 2024 Oct 1;278:126526. doi: 10.1016/j.talanta.2024.126526. Epub 2024 Jul 8.

Abstract

Understanding charge transport in metal ion-mediated glutathione-stabilized gold nanoclusters (GSH-Au NCs) has proved difficult due to the presence of various competitive mechanisms, such as electron transfer (ET) and aggregation induction effect (AIE). In this paper, we present a dual-channel fluorescence (FL) and second-order Rayleigh scattering (SRS) sensing method for high-throughput classification of metal ions, relying on the competition between ET and AIE using GSH-Au NCs. The SRS signals show significant enhancement when Pb, Ag, Al, Cu, Fe, and Hg are present, as a result of the aggregation of GSH-Au NCs. Notably, the fluorescence signal exhibits the opposite trend. The FL intensities of GSH-Au NCs are enhanced by Pb, Ag, and Al through the AIE mechanism, while they are quenched by Cu, Fe, and Hg, which is dominated by the ET mechanism. By employing principal component analysis and hierarchical cluster analysis, these signals are transformed into unique fingerprints and Euclidean distances, respectively, enabling successful distinction of six metal ions and their mixtures with a low detection limit of 30 nM. This new strategy has successfully addressed interference from impurities in the testing of real water samples, demonstrating its strong ability to detect multiple metal ions. Impressively, we have achieved molecular cryptosteganography, which involves encoding, storing, and concealing information by transforming the selective response of GSH-Au NCs to binary strings. This research is anticipated to advance utilization of nanomaterials in logic sensing and information safety, bridging the gap between molecular sensors and information systems.

摘要

由于存在各种竞争机制,如电子转移(ET)和聚集诱导效应(AIE),理解金属离子介导的谷胱甘肽稳定的金纳米团簇(GSH-Au NCs)中的电荷传输已被证明是困难的。在本文中,我们提出了一种双通道荧光(FL)和二阶瑞利散射(SRS)传感方法,用于金属离子的高通量分类,该方法依赖于利用GSH-Au NCs的ET和AIE之间的竞争。当存在Pb、Ag、Al、Cu、Fe和Hg时,由于GSH-Au NCs的聚集,SRS信号显著增强。值得注意的是,荧光信号呈现相反的趋势。GSH-Au NCs的FL强度通过AIE机制被Pb、Ag和Al增强,而被Cu、Fe和Hg淬灭,这主要由ET机制主导。通过采用主成分分析和层次聚类分析,这些信号分别被转换为独特的指纹和欧几里得距离,从而能够成功区分六种金属离子及其混合物,检测限低至30 nM。这种新策略成功解决了实际水样检测中杂质的干扰,证明了其检测多种金属离子的强大能力。令人印象深刻的是,我们实现了分子隐写术,即通过转换GSH-Au NCs对二进制字符串的选择性响应来编码、存储和隐藏信息。预计这项研究将推动纳米材料在逻辑传感和信息安全中的应用,弥合分子传感器与信息系统之间的差距。

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