A new class of porous silicon electrochemical transducers built from pyrolyzed polyfurfuryl alcohol

IF 8.1 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Anandapadmanabhan A. Rajendran, Keying Guo, Alberto Alvarez-Fernandez, Thomas R. Gengenbach, Marina B. Velasco, Maximiliano J. Fornerod, Kandeel Shafique, Máté Füredi, Pilar Formentín, Hedieh Haji-Hashemi, Stefan Guldin, Nicolas H. Voelcker, Xavier Cetó, Beatriz Prieto-Simón
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Abstract

Carbon-based nanomaterials are key to developing high-performing electrochemical sensors with improved sensitivity and selectivity. Nonetheless, limitations in their fabrication and integration into devices often constrain their practical applications. Moreover, carbon nanomaterials-based electrochemical devices still face problems such as large background currents, poor stability, and slow kinetics. To advance towards a new class of carbon nanostructured electrochemical transducers, we propose the in-situ polymerization and carbonization of furfuryl alcohol (FA) on porous silicon (pSi) to produce a tailored and highly stable transducer. The thin layer of polyfurfuryl alcohol (PFA) that conformally coats the pSi scaffold transforms into nanoporous carbon when subjected to pyrolysis above 600 °C. The morphological and chemical properties of PFA-pSi were characterized by scanning electron microscopy, and Raman and X-ray photoelectron spectroscopies. Their stability and electrochemical performance were investigated by cyclic voltammetry and electrochemical impedance spectroscopy in [Fe(CN)6]3-/4-, [Ru(NH3)6]2+/3+, and hydroquinone. PFA-pSi showed superior electrochemical performance compared to screen-printed carbon electrodes while also surpassing glassy carbon electrodes in specific aspects. Besides, PFA-pSi has the additional advantage of easy tuning of the electroactive surface area. To prove its potential for biosensing purposes, a DNA sensor based on quantifying the partial pore blockage of the pSi upon target hybridization was built on PFA-pSi. The sensor showed a limit of detection of 1.4 pM, outperforming other sensors based on the same sensing mechanism.

Abstract Image

由热解聚糠醇制成的新型多孔硅电化学传感器
碳基纳米材料是开发具有更高灵敏度和选择性的高性能电化学传感器的关键。然而,碳基纳米材料在制造和集成到设备中的局限性往往会限制其实际应用。此外,基于碳纳米材料的电化学装置仍然面临着背景电流大、稳定性差和动力学速度慢等问题。为了推动新型碳纳米结构电化学换能器的发展,我们提出了在多孔硅(pSi)上对糠醇(FA)进行原位聚合和碳化,从而制备出一种量身定制且高度稳定的换能器。在 600 °C 以上的高温分解过程中,覆盖在多孔硅支架上的聚糠醇 (PFA) 薄层会转化为纳米多孔碳。扫描电子显微镜、拉曼光谱和 X 射线光电子能谱对 PFA-pSi 的形态和化学特性进行了表征。在[Fe(CN)6]3-/4-、[Ru(NH3)6]2+/3+和对苯二酚中,通过循环伏安法和电化学阻抗谱研究了它们的稳定性和电化学性能。与丝网印刷碳电极相比,PFA-pSi 显示出更优越的电化学性能,同时在某些方面还超过了玻璃碳电极。此外,PFA-pSi 还具有易于调节电活性表面积的优势。为了证明 PFA-pSi 在生物传感方面的潜力,我们在 PFA-pSi 上构建了一个 DNA 传感器,该传感器基于目标杂交时 pSi 部分孔隙堵塞情况的量化。该传感器的检测限为 1.4 pM,优于基于相同传感机制的其他传感器。
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来源期刊
Materials Today Advances
Materials Today Advances MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
14.30
自引率
2.00%
发文量
116
审稿时长
32 days
期刊介绍: Materials Today Advances is a multi-disciplinary, open access journal that aims to connect different communities within materials science. It covers all aspects of materials science and related disciplines, including fundamental and applied research. The focus is on studies with broad impact that can cross traditional subject boundaries. The journal welcomes the submissions of articles at the forefront of materials science, advancing the field. It is part of the Materials Today family and offers authors rigorous peer review, rapid decisions, and high visibility.
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