Study of surface modification strategies to create glassy carbon-supported, aptamer-based sensors for continuous molecular monitoring.
Study of surface modification strategies to create glassy carbon-supported, aptamer-based sensors for continuous molecular monitoring.
复制标题
研究表面改性策略，以创建用于连续分子监测的玻碳支撑的适体传感器。
DOI：
10.1007/s00216-022-04015-5
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发表时间：
2022-07
影响因子：
4.3
通讯作者：
Arroyo-Curras, Netzahualcoyotl
中科院分区：
文献类型：
--
作者：
Pellitero, Miguel Aller;Arroyo-Curras, Netzahualcoyotl
关键词：
基于适配体的电化学（E-AB）传感器独特地实现了生物流体中的无试剂、可逆和连续的分子监测。由于这种能力，E-AB传感器已被提出用于治疗药物监测。然而，为了实现从实验室到临床的转换，理想情况下，E-AB传感器应可靠地连续运行数天。相反，因为这些传感器通常是通过易于从电极表面解吸的烷硫醇的自组装在金表面上制造的，所以它们在短短几个小时内就会经历显著的信号损失。为了克服这个问题，我们的团队正试图将E-AB传感器接口从硫醇-金组装迁移到更强的共价键。在这里，我们探讨了碳电极作为E-AB传感器的替代基板的修改。我们研究了三种策略来功能化碳表面：（I）阳极氧化产生表面羧基，（II）电接枝的arenedazionium离子，和（III）电接枝的脂肪族伯胺。我们的研究结果表明，脂肪族伯胺的电接枝是唯一的策略，实现单层组织和包装密度密切可比的烷硫醇金。此外，所得单层能够共价束缚DNA适体，并支持小分子靶标或互补DNA链的电化学传感。当使用正电压扫描窗口时，相对于基准硫醇-金单层，这些单层在生物流体中的连续伏安询问下也实现了上级稳定性。基于这些结果，我们假设脂肪族伯胺的电接枝作为开发具有增加的操作稳定性的碳支撑的E-AB传感器的前进路径。在线版本包含补充材料，可通过10.1007/s 00216 -022-04015-5获得。
Electrochemical, aptamer-based (E-AB) sensors uniquely enable reagentless, reversible, and continuous molecular monitoring in biological fluids. Because of this ability, E-AB sensors have been proposed for therapeutic drug monitoring. However, to achieve translation from the bench to the clinic, E-AB sensors should ideally operate reliably and continuously for periods of days. Instead, because these sensors are typically fabricated on gold surfaces via self-assembly of alkanethiols that are prone to desorption from electrode surfaces, they undergo significant signal losses in just hours. To overcome this problem, our group is attempting to migrate E-AB sensor interfaces away from thiol-on-gold assembly towards stronger covalent bonds. Here, we explore the modification of carbon electrodes as an alternative substrate for E-AB sensors. We investigated three strategies to functionalize carbon surfaces: (I) anodization to generate surface carboxylic groups, (II) electrografting of arenediazonium ions, and (III) electrografting of primary aliphatic amines. Our results indicate that electrografting of primary aliphatic amines is the only strategy achieving monolayer organization and packing densities closely comparable to those obtained by alkanethiols on gold. In addition, the resulting monolayers enable covalent tethering of DNA aptamers and support electrochemical sensing of small molecule targets or complimentary DNA strands. These monolayers also achieve superior stability under continuous voltammetric interrogation in biological fluids relative to benchmark thiol-on-gold monolayers when a positive voltage scan window is used. Based on these results, we postulate the electrografting of primary aliphatic amines as a path forward to develop carbon-supported E-AB sensors with increased operational stability. The online version contains supplementary material available at 10.1007/s00216-022-04015-5.
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