Substituent Effects Impact Surface Charge and Aggregation of Thiophenol-Labeled Gold Nanoparticles for SERS Biosensors.
Substituent Effects Impact Surface Charge and Aggregation of Thiophenol-Labeled Gold Nanoparticles for SERS Biosensors.
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DOI：
10.3390/bios12010025
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发表时间：
2022-01-05
期刊：
影响因子：
--
通讯作者：
Batra SK
中科院分区：
文献类型：
--
作者：
File N;Carmicheal J;Krasnoslobodtsev AV;Japp NC;Souchek JJ;Chakravarty S;Hollingsworth MA;Sasson AA;Natarajan G;Kshirsagar PG;Jain M;Hayashi C;Junker WM;Kaur S;Batra SK
Sers免疫分析生物传感器由于其高灵敏度和对多标记面板的日益关注而在临床诊断方面具有巨大的潜力。然而，他们的发展一直受到阻碍的困难，在设计兼容的外来拉曼标签。先前的研究主要集中在选择用于多路复用的拉曼报告分子（RRM）的光谱特性上，因为良好区分的光谱的存在对于同时检测是必不可少的。然而，尽管这些候选物与其他有效的RRM相似，但它们通常会诱导用作Sers纳米标签的金纳米颗粒的聚集。因此，需要更好地理解影响RRM涂覆的金纳米颗粒聚集的因素。取代基电子效应对粒子稳定性进行了研究，使用各种对位取代的硫酚。官能团修饰的诱导和共振效应与纳米颗粒表面电荷以及它们的稳定性密切相关。用硫酚处理减少了柠檬酸盐稳定的金纳米颗粒的负表面电荷，但吸电子取代基限制了这种减少的幅度。有人提出，这种现象是通过影响竞争硫结合模式的相互作用而产生的。这对使用硫醇修饰的金表面设计生物传感器具有广泛的影响。根据这些发现，使用具有最多吸电子取代基的两种苯硫酚化合物：NO2和CN，设计了概念验证的多重Sers生物传感器。
SERS immunoassay biosensors hold immense potential for clinical diagnostics due to their high sensitivity and growing interest in multi-marker panels. However, their development has been hindered by difficulties in designing compatible extrinsic Raman labels. Prior studies have largely focused on spectroscopic characteristics in selecting Raman reporter molecules (RRMs) for multiplexing since the presence of well-differentiated spectra is essential for simultaneous detection. However, these candidates often induce aggregation of the gold nanoparticles used as SERS nanotags despite their similarity to other effective RRMs. Thus, an improved understanding of factors affecting the aggregation of RRM-coated gold nanoparticles is needed. Substituent electronic effects on particle stability were investigated using various para-substituted thiophenols. The inductive and resonant effects of functional group modifications were strongly correlated with nanoparticle surface charge and hence their stability. Treatment with thiophenols diminished the negative surface charge of citrate-stabilized gold nanoparticles, but electron-withdrawing substituents limited the magnitude of this diminishment. It is proposed that this phenomenon arises by affecting the interplay of competing sulfur binding modes. This has wide-reaching implications for the design of biosensors using thiol-modified gold surfaces. A proof-of-concept multiplexed SERS biosensor was designed according to these findings using the two thiophenol compounds with the most electron-withdrawing substitutions: NO2 and CN.
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